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Radiation Detection Concepts Methods and Devices

The document is a comprehensive guide on radiation detection, covering concepts, methods, and devices related to the field. It includes historical context, basic atomic and nuclear physics, radiation interactions, and various sources of radiation. The book serves as a resource for understanding the principles and applications of radiation detection technology.
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© © All Rights Reserved
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0% found this document useful (0 votes)
254 views1,313 pages

Radiation Detection Concepts Methods and Devices

The document is a comprehensive guide on radiation detection, covering concepts, methods, and devices related to the field. It includes historical context, basic atomic and nuclear physics, radiation interactions, and various sources of radiation. The book serves as a resource for understanding the principles and applications of radiation detection technology.
Copyright
© © All Rights Reserved
We take content rights seriously. If you suspect this is your content, claim it here.
Available Formats
Download as PDF, TXT or read online on Scribd
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Radiation Detection

Concepts, Methods, and Devices


Douglas S. McGregor
J. Kenneth Shultis
Radiation Detection
Radiation Detection
Concepts, Methods, and Devices

Douglas S. McGregor
J. Kenneth Shultis
First edition published 2020
by CRC Press
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and by CRC Press


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c 2021 Taylor & Francis Group, LLC

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Library of Congress Cataloging-in-Publication Data


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ISBN: 978-1-4398-1939-5 (hbk)


ISBN: 978-1-4398-1940-1 (ebk)

Typeset in CMR
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Visit the Taylor & Francis Web site at


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and the CRC Press Web site at


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To the countless pioneers, inventors and scholars
whose seminal contributions have developed
radiation detection into a mature discipline
About the Cover Picture

A 1960 image from CERN’s first liquid hydrogen bubble


chamber, which was 32 cm in diameter. Here 16-GeV
negative pions enter from the left and are seen as the
horizontal bubble trails. One pion interacts with a proton
in the liquid hydrogen producing a spray of new particles
including a neutral Λ0 that quickly decays into a proton
and negative pion to produce the sideway “V” (slightly
left of center). Lower energy charged particles produced
in the original and subsequent interactions create spiral
tracks in the magnetic field of the chamber. Photograph
courtesy of CERN.
Contents

Preface xxi

About the Authors xxv

1 Origins 1
1.1 A Brief History of Radiation Discovery 1
1.2 A Brief History of Radiation Detectors 10

2 Introduction to Nuclear Instrumentation 19


2.1 Introduction 19
2.2 The Detector 20
2.3 Nuclear Instrumentation 21
2.4 History of NIM Development 21
2.5 NIM Components 23
2.5.1 The NIM Bin 23
2.5.2 Detector Power Supplies 24
2.5.3 Preamplifier 26
2.5.4 Amplifier 27
2.5.5 Oscilloscope 27
2.5.6 Pulse Discriminators 27
2.5.7 Counter/Timer 28
2.5.8 Pulse Generator 28
2.5.9 Coincidence Modules 28
2.5.10 Time-to-Amplitude Converters 29
2.5.11 Analog-to-Digital Converters 29
2.5.12 Photomultiplier Tube Base 29
2.5.13 Multichannel Analyzer 29
2.5.14 Other NIM Components 30
2.6 CAMAC 31
2.7 Nuclear Instruments other than NIM or CAMAC 31

vii
viii Contents

2.8 Cables and Connectors 31


2.8.1 Cables 32
2.8.2 Delay Lines 33
2.8.3 Connectors 33

3 Basic Atomic and Nuclear Physics 37


3.1 Modern Physics Concepts 37
3.1.1 The Special Theory of Relativity 37
3.1.2 Principle of Relativity 38
3.1.3 Results of the Special Theory of Relativity 39
3.2 Highlights in the Evolution of Atomic Theory 41
3.2.1 Radiation as Waves and Particles 42
3.2.2 Early Observations 42
3.2.3 The Photoelectric Effect 42
3.2.4 Compton Scattering 44
3.2.5 Electromagnetic Radiation: Wave-Particle Duality 45
3.2.6 Electron Scattering 46
3.3 Development of the Modern Atom Model 47
3.3.1 Discovery of Radioactivity 47
3.3.2 Thomson’s Atomic Model: The Plum Pudding Model 48
3.3.3 The Rutherford Atomic Model 49
3.3.4 The Bohr Atomic Model 49
3.3.5 Extension of the Bohr Theory: Elliptic Orbits 52
3.3.6 The Quantum Mechanical Model of the Atom 53
3.3.7 Wave-Particle Duality 54
3.4 Quantum Mechanics 54
3.4.1 Schrödinger’s Wave Equation 54
3.4.2 The Wave Function 55
3.4.3 The Uncertainty Principle 56
3.4.4 Particle in a Potential Well 56
3.4.5 The Hydrogen Atom 60
3.4.6 Energy Levels for Multielectron Atoms 62
3.4.7 Success of Quantum Mechanics 64
3.5 The Fundamental Constituents of Ordinary Matter 64
3.5.1 Dark Matter and Energy 66
3.5.2 Atomic and Nuclear Nomenclature 67
3.5.3 Relative Atomic Masses 68
3.5.4 The Atomic Mass Unit 68
3.5.5 Avogadro’s Number 69
3.5.6 Mass of an Atom 69
3.5.7 Number Density of Atoms and Isotopes 69
3.5.8 Size of an Atom 70
3.5.9 Nuclear Dimensions 70
3.6 Nuclear Reactions 71
3.6.1 Q-Value for a Reaction 71
3.6.2 Conservation of Charge and the Calculation of Q-Values 72
3.6.3 Special Case for Changes in the Proton Number 73
Contents ix

3.7 Radioactivity 73
3.7.1 Types of Radioactive Decay 74
3.7.2 Radioactive Decay Diagrams 74
3.7.3 Energetics of Radioactive Decay 76
3.7.4 Exponential Decay 84
3.7.5 The Half-Life 85
3.7.6 Decay Probability for a Finite Time Interval 85
3.7.7 Mean Lifetime 86
3.7.8 Activity 86
3.7.9 Decay by Competing Processes 87
3.7.10 Decay Dynamics 87

4 Radiation Interactions 93
4.1 Introduction 93
4.2 Indirectly Ionizing Radiation 93
4.2.1 Attenuation of Neutral Particle Beams 93
4.2.2 The Linear Interaction Coefficient 94
4.2.3 Attenuation of Uncollided Radiation 95
4.2.4 Average Travel Distance Before an Interaction 96
4.2.5 Half-Thickness 96
4.2.6 Microscopic Cross Sections 96
4.2.7 Calculation of Radiation Interaction Rates 97
4.3 Scattering Interactions 99
4.3.1 Differential Scattering Coefficients 99
4.3.2 Conservation Laws for Scattering Reactions 100
4.3.3 Scattering of Photons by Free Electrons 101
4.3.4 Scattering of Neutrons by Atomic Nuclei 102
4.3.5 Threshold Energies for Neutron Inelastic Scattering 103
4.3.6 Neutron Scattering in the Center-of-Mass System 104
4.3.7 Limiting Cases in Classical Mechanics of Elastic Scattering 105
4.3.8 Relativistic Elastic Scattering of Electrons and Heavy Charged Particles 106
4.4 Photon Cross Sections 106
4.4.1 Thomson Cross Section for Incoherent Scattering 107
4.4.2 Klein-Nishina Cross Section for Incoherent Scattering 107
4.4.3 Incoherent Scattering Cross Sections for Bound Electrons 112
4.4.4 Coherent (Rayleigh) Scattering 112
4.4.5 Photoelectric Effect 112
4.4.6 Pair Production 114
4.4.7 Photon Interactions—Minor Effects 115
4.4.8 Photon Attenuation Coefficients 116
4.5 Neutron Interactions 116
4.5.1 Classification of Types of Interactions 117
4.5.2 Thermal Neutron Interactions 121
4.5.3 Neutron Differential Scattering Cross Sections 123
4.5.4 Average Energy Transfer in Neutron Scattering 124
4.5.5 Radiative Capture of Neutrons 125
4.5.6 Neutron-Induced Fission 126
x Contents

4.6 Charged-Particle Interactions 126


4.6.1 Collisional Energy Loss 127
4.6.2 Radiative Energy Loss 130
4.6.3 Estimating Charged-Particle Ranges 131
4.6.4 Electron Energy Loss and Range 132
4.6.5 Spatial Distribution of the Electron Energy Absorption 136
4.6.6 Heavy Charged-Particle Energy Loss 139
4.6.7 Heavy Charged-Particle Range 140
4.6.8 The Bragg Curve 143
4.6.9 Approximate Range Formula for Charged Particles 144
4.6.10 Range of Fission Fragments 147

5 Sources of Radiation 153


5.1 Introduction 153
5.1.1 Origins of Ionizing Radiation 153
5.1.2 Physical Characterization of Radiation Sources 154
5.2 Sources of Gamma Rays 154
5.2.1 Naturally Occurring Radionuclides 155
5.2.2 Prompt Fission Gamma Photons 157
5.2.3 Fission-Product Gamma Photons 157
5.2.4 Capture Gamma Photons 158
5.2.5 Inelastic Scattering Gamma Photons 159
5.2.6 Activation Gamma Photons 159
5.2.7 Positron Annihilation Photons 159
5.3 Sources of X Rays 159
5.3.1 Characteristic X Rays 161
5.3.2 Bremsstrahlung 163
5.3.3 X-Ray Machines 166
5.3.4 Synchrotron X Rays 168
5.4 Sources of Neutrons 168
5.4.1 Fission Neutrons 168
5.4.2 Fusion Neutrons 169
5.4.3 Photoneutrons 170
5.4.4 Alpha-Neutron Sources 172
5.4.5 Activation Neutrons 173
5.4.6 Spallation Neutron Sources 173
5.5 Sources of Charged Particles 174
5.5.1 Beta Decay 174
5.5.2 Alpha Decay 176
5.5.3 Photon Interactions 177
5.5.4 Neutron Interactions 178
5.5.5 Accelerators 179
5.6 Cosmic Rays 179
5.6.1 High Energy Gamma Rays 180
Contents xi

6 Probability and Statistics for Radiation Counting 183


6.1 Introduction 183
6.1.1 Types of Measurement Uncertainties 184
6.1.2 Probability and Statistics 184
6.2 Probability and Cumulative Distribution Functions 185
6.2.1 Continuous Random Variable 185
6.2.2 Discrete Random Variable 185
6.3 Mode, Mean and Median 185
6.3.1 Mode 186
6.3.2 Mean 186
6.3.3 Median 187
6.4 Variance and Standard Deviation of a PDF 187
6.5 Probability Data Distribution 188
6.5.1 Sample Mean 189
6.5.2 Sample Median 191
6.5.3 Trimmed Sample Mean 193
6.5.4 Sample Variance 194
6.6 Binomial Distribution 196
6.6.1 Radioactive Decay and the Binomial Distribution 199
6.7 Poisson Distribution 200
6.8 Gaussian or Normal Distribution 204
6.8.1 Standard Normal Distribution 207
6.8.2 Cumulative Normal Distribution and the Error Function 209
6.8.3 Discrete Gaussian Distribution 211
6.8.4 The Normal Distribution in Radiation Measurements 212
6.9 Error Propagation 214
6.9.1 A Measurement is Scaled by a Constant 217
6.9.2 Random Variables are Added or Subtracted 218
6.9.3 Random Variables are Multiplied or Divided 219
6.9.4 Random Variables in Exponents or Logarithms 221
6.9.5 A Series of Radiation Measurements 222
6.9.6 Measurements Over Different Time Intervals 224
6.9.7 Caution about Error Propagation 227
6.10 Data Interpretation 227
6.10.1 Radiation Detection Limits 229
6.10.2 Chi-Square Test for “Goodness” of Data 233
6.10.3 Presentation of Data 236
6.10.4 Concluding Remarks 238

7 Source and Detector Effects 243


7.1 Detector Efficiency 243
7.2 Source Effects 245
7.2.1 Alpha Particles 246
7.2.2 Beta Particles 250
7.2.3 Penetrating Radiations (γ rays, x rays, neutrons) 253
7.2.4 Source Decay During Measurement 253
7.2.5 Contamination 254
xii Contents

7.3 Detector Effects 254


7.3.1 Scattering and Absorption by the Detector Window 254
7.3.2 Time Interval Distribution between Radioactive Decays 255
7.3.3 Dead Time 255
7.3.4 Models for Dead Time 257
7.3.5 Counting Error Associated with Dead Time 260
7.3.6 Methods for Measuring Dead Time 261
7.4 Geometric Effects: View Factors 267
7.4.1 Point Isotropic Sources 268
7.4.2 Isotropic Area Sources 272
7.4.3 Monte Carlo Approach to View Factor Angle Calculations 274
7.5 Geometric Corrections: Detector Parallax Effects 274
7.5.1 Attenuation and Scattering Effects Outside the Detector 276

8 Essential Electrostatics 281


8.1 Electric Field 281
8.1.1 Alternate Derivation of Gauss’ Law 284
8.2 Electrical Potential Energy 284
8.3 Capacitance 286
8.4 Current and Stored Energy 287
8.5 Basics of Charge Induction 288
8.5.1 Green’s Reciprocation Theorem 290
8.6 Charge Induction for a Planar Detector 290
8.6.1 Planar Detector with Stationary Space Charge 294
8.6.2 A Planar Detector Composed of Two Materials 298
8.7 Charge Induction for a Cylindrical Detector 300
8.8 Charge Induction for Spherical and Hemispherical Detectors 301
8.9 Concluding Remarks 303

9 Gas-Filled Detectors: Ion Chambers 305


9.1 General Operation 305
9.2 Electrons and Ions in Gas 307
9.2.1 Ionization 307
9.2.2 Diffusion Effects 309
9.2.3 Electron and Ion Transport 312
9.2.4 Charge Transfer 317
9.2.5 Electron Attachment 318
9.3 Recombination 321
9.3.1 Columnar Recombination 321
9.3.2 Volumetric Recombination 323
9.3.3 Preferential Recombination 329
9.4 Ion Chamber Operation 330
9.4.1 Planar Ion Chambers 331
9.4.2 Coaxial Ion Chambers 337
9.5 Ion Chamber Designs 340
9.5.1 Basic Designs and Characteristics 341
9.5.2 Gamma-Ray Ion Chamber Designs 343
9.5.3 Neutron-Sensitive Ion Chambers 344
Contents xiii

9.5.4 Compensated Ion Chambers 344


9.5.5 Frisch Grid Ion Chambers 345
9.5.6 Free Air Ion Chambers 346
9.5.7 Pocket Ion Chambers 347
9.5.8 Cloud Chambers 348
9.5.9 Smoke Detector Ionization Chambers 351
9.6 Summary 351

10 Gas-Filled Detectors: Proportional Counters 355


10.1 Introduction 355
10.2 General Operation 356
10.3 Townsend Avalanche Multiplication 357
10.3.1 The Rose-Korff Formula for M 358
10.3.2 The Diethorn Formula for M 362
10.3.3 The Zastawny Formula for M 363
10.3.4 The Kowalski Formula for M 364
10.4 Gas Dependence 364
10.4.1 Quenching Gas 365
10.4.2 Penning Mixtures 367
10.5 Proportional Counter Operation 368
10.5.1 Pulse Shape 369
10.5.2 Space Charge Effects 373
10.5.3 Counting Curve 373
10.5.4 Fluctuations of the Gas Multiplication Process 377
10.6 Selected Proportional Counter Variations 386
10.6.1 Gas-Flow Proportional Counters 386
10.6.2 Sealed Proportional Counters 389
10.6.3 Proportional Counters for Low Energy Gamma-Rays 390
10.6.4 Position Sensitive Proportional Counters 391
10.6.5 Multiwire Proportional Counters 392
10.6.6 Microstrip Gas Chambers 394
10.6.7 Straw Tubes 396
10.6.8 Gas Electron Multiplier 397
10.6.9 Neutron-Sensitive Proportional Counters 397
10.6.10 Selected Planar Proportional Counters 398

11 Gas-Filled Detectors: Geiger-Müller Counters 403


11.1 Geiger Discharge 403
11.2 Basic Design 404
11.3 Fill Gases 406
11.3.1 Quenching 407
11.4 Pulse Shape 410
11.4.1 Dead, Resolving, and Recovery Times 411
11.5 Radiation Measurements 412
11.5.1 Counting Plateau 412
11.5.2 Alpha and Beta Particle Counting 414
11.5.3 Gamma-Ray Detection 415
xiv Contents

11.6 Special G-M Counter Designs 416


11.7 Commercial G-M Counters 417

12 Review of Solid State Physics 423


12.1 Introduction 423
12.2 Solid State Physics 423
12.2.1 Crystals and Periodic Lattices 423
12.2.2 Bravais Lattice 424
12.2.3 Miller Indices 426
12.2.4 Reciprocal Lattice 429
12.2.5 Energy Band Gap 430
12.3 Quantum Mechanics 432
12.3.1 Potential Barriers 432
12.3.2 Kronig-Penney Model 436
12.4 Semiconductor Physics 438
12.4.1 Brillouin Zones 438
12.4.2 Effective Mass 439
12.5 Charge Transport 449
12.5.1 Charge Carrier Mobility 456
12.5.2 Material Resistivity and Capacity 457
12.5.3 Intrinsic Semiconductors 458
12.5.4 Impurities and Extrinsic Semiconductors 465
12.6 Summary 478

13 Scintillation Detectors and Materials 481


13.1 Scintillation Detectors 481
13.2 Inorganic Scintillators 482
13.2.1 Theory of Scintillation for Inorganic Scintillators 485
13.2.2 General Properties of Inorganic Scintillators 489
13.2.3 Properties of Several Common Inorganic Scintillators 502
13.3 Organic Scintillators 522
13.3.1 Theory of Scintillation for Organic Scintillators 523
13.3.2 Organic Crystalline Scintillators 532
13.3.3 Liquid Scintillators 537
13.3.4 Plastic Scintillators 546
13.4 Gaseous Scintillators 548
13.4.1 Development of Gas Scintillator Counters 549
13.4.2 Theory of Gas Scintillation Counters 550
13.4.3 Factors Affecting Performance 551
13.4.4 Mixtures of Noble Gases 552
13.4.5 Liquid and Solid Noble Elements 553
13.4.6 Gas Proportional Scintillation Counters 554

14 Light Collection Devices 565


14.1 Photomultiplier Tubes 565
14.1.1 Basic Design 567
14.1.2 Light Collection and Coupling 568
Contents xv

14.1.3 Photocathode Materials and Design 575


14.1.4 Dynode Materials 586
14.1.5 PMT Dynode Designs and Configurations 593
14.1.6 Gain 599
14.1.7 Factors Affecting the Performance of a PMT 600
14.1.8 Ancillary Equipment 607
14.1.9 Environmental Effects 611
14.2 Semiconductor Photodetectors 611
14.2.1 Photodiodes 612
14.2.2 Drift Diodes 616
14.2.3 Avalanche Diodes 617
14.2.4 Semiconductor Photomultipliers 621

15 Basics of Semiconductor Detector Devices 627


15.1 Introduction 627
15.2 Charge Carrier Collection 627
15.2.1 Charge Carrier Generation, Recombination and Injection 628
15.2.2 Radiative Recombination 628
15.2.3 Shockley-Read-Hall Recombination 629
15.2.4 Equations of Continuity 631
15.3 Basic Semiconductor Detector Configurations 634
15.3.1 The pn Junction 635
15.3.2 pin Junction Devices 645
15.3.3 Metal-Semiconductor Contacts 646
15.3.4 The MOS Structure 658
15.3.5 Ohmic Contacts 663
15.3.6 Series Resistance and Space Charge Effects 665
15.3.7 Resistive and Photoconductive Devices 668
15.3.8 Photon Drag Detectors 670
15.4 Measurements of Semiconductor Detector Properties 671
15.4.1 IV Measurements 671
15.4.2 CV Measurements 673
15.4.3 Measurement of Contact Resistance 675
15.4.4 Measurement of Resistivity 677
15.4.5 Measurement of Charge Carrier Mobility 679
15.4.6 Measurement of the μτ Product 682
15.5 Charge Induction 684
15.5.1 Charge Induction With Trapping 684
15.5.2 Energy Resolution Improvement Methods and Designs 690

16 Semiconductor Detectors 705


16.1 Introduction 705
16.2 General Semiconductor Properties 707
16.2.1 Atomic Numbers and Mass Density 708
16.2.2 Band Gap 709
16.2.3 Ionization Energy 710
16.2.4 Mobility 713
xvi Contents

16.2.5 Resistivity 716


16.2.6 Mean Free Drift Time 717
16.2.7 Linearity 717
16.3 Semiconductor Detector Applications 719
16.3.1 Charged Particle Detectors 719
16.3.2 Gamma-Ray and X-Ray Detectors 719
16.3.3 Neutron Detectors 721
16.4 Detectors Based on Group IV Materials 722
16.4.1 Detectors Based on Silicon 722
16.4.2 Detectors Based on Ge 747
16.4.3 Diamond Detectors 765
16.5 Compound Semiconductor Detectors 767
16.5.1 SiC Detectors 769
16.5.2 Detectors Based on Group III-V Materials 771
16.5.3 Detectors Based on Group II-VI Materials 777
16.5.4 Detectors Based on Halide Compounds 787
16.6 Additional Semiconductors of Interest 793
16.7 Summary 797

17 Slow Neutron Detectors 813


17.1 Cross Sections in the 1/v Region 813
17.2 Slow Neutron Reactions Used for Neutron Detection 815
17.2.1 The 3 He Reaction 816
17.2.2 The 10 B Neutron Reaction 817
17.2.3 The 6 Li Neutron Reaction 818
17.2.4 The 155 Gd and 157 Gd Neutron Reactions 819
17.2.5 The 113 Cd Neutron Reaction 820
17.2.6 The 199 Hg Neutron Reaction 820
17.2.7 Fission Reactions 821
17.3 Gas-Filled Slow Neutron Detectors 822
17.3.1 Detectors with Neutron Absorbing Fill Gases 822
17.3.2 Detectors with Neutron Reactive Coatings and Layers 829
17.4 Scintillator Slow Neutron Detectors 848
17.4.1 Neutron Reactive Scintillators 848
17.4.2 Scintillators Loaded with Neutron Reactive Materials 851
17.5 Semiconductor Slow Neutron Detectors 855
17.5.1 Bulk Semiconductor Neutron Detectors 859
17.6 Neutron Diffraction 861
17.6.1 The Structure Factor for Crystals F hkl 863
17.6.2 Angular Response to a Maxwellian Neutron Distribution 864
17.6.3 Measurements with Diffracted Neutron Beams 865
17.7 Calibration of Slow Neutron Detectors 866
17.7.1 Method of the NIST 866
17.7.2 Method of Reuter Stokes 867
17.7.3 Method of ORNL 867
17.7.4 Method of Sampson and Vincent 867
17.7.5 Method of McGregor and Shultis 868
Contents xvii

17.8 Neutron Detection by Foil Activation 870


17.8.1 Cadmium Ratio 874
17.8.2 Measuring Activation Rates 875
17.8.3 Flux Correction Factors 876
17.8.4 Correction for Non-1/v Absorption 877
17.8.5 Correction for Cadmium Filter Effects 877
17.8.6 Correction for Flux Perturbation and Self-Shielding 878
17.9 Self-Powered Neutron Detectors 881
17.10 Time-of-Flight Methods 887

18 Fast Neutron Detectors 897


18.1 Detection Mechanisms 897
18.1.1 Neutron Moderation and Scattering 897
18.1.2 Multiscattered Neutrons 898
18.1.3 Absorption 899
18.2 Detectors Based on Moderation 899
18.2.1 Bonner Spheres 899
18.2.2 REM Counters 904
18.2.3 Long Counter 907
18.2.4 Directional Neutron Spectrometer 909
18.2.5 Other Moderated Detectors 910
18.3 Detectors Based on Recoil Scattering 910
18.3.1 Gas Detectors Based on Recoil Scattering 913
18.3.2 Unfolding the Recoil Energy Spectrum 918
18.3.3 Scintillators Used in Recoil Neutron Scattering 919
18.4 Semiconductor Fast Neutron Detectors 931
18.5 Detectors Based on Absorption Reactions 933
18.5.1 3 He Detectors 933
18.5.2 6 LiI:Eu Scintillators 935
18.5.3 6 Li Sandwich 936
18.5.4 The Grey Detector 938
18.5.5 Cryogenic Detectors 938
18.5.6 Foil Activation Methods 939
18.5.7 The Foil Inversion Problem 940
18.6 Summary 942

19 Luminescent and Additional Detectors 949


19.1 Luminescent Dosimeters 949
19.1.1 Thermoluminescent Dosimeters 949
19.1.2 Optically Stimulated Luminescent Dosimeters 973
19.2 Photographic Film 984
19.2.1 Basics of Photographic Film 985
19.2.2 Photographic Film Characteristics 986
19.2.3 Film Dosimetry Badges 990
19.3 Track Detectors 991
19.3.1 Nuclear Track Emulsions 991
19.3.2 Track Etch Detectors 993
xviii Contents

19.3.3 Spark Chambers 1001


19.3.4 Bubble Chambers 1002
19.3.5 Superheated Drop Detectors 1004
19.4 Cryogenic Detectors 1007
19.4.1 Methods of Cooling 1008
19.4.2 Cryogenic Microcalorimeters 1009
19.4.3 Athermal Cryogenic Charge Detectors 1016
19.5 Wavelength-Dispersive Spectroscopy 1020
19.6 Čerenkov (Cherenkov) Detectors 1021

20 Radiation Measurements and Spectroscopy 1035


20.1 Introduction 1035
20.2 Basic Concepts 1036
20.3 Detector Response Models 1038
20.4 Gamma-Ray Spectroscopy 1040
20.4.1 Gamma-Ray and X-Ray Spectral Features 1041
20.4.2 Spectral Response Function 1051
20.4.3 Qualitative Analysis 1051
20.4.4 Quantitative Analysis 1052
20.4.5 Area Under an Isolated Peak 1053
20.4.6 Linear Least Squares Method for a Straight Line 1054
20.4.7 General Linear Least-Squares Model Fitting 1057
20.4.8 Non-Linear Least-Squares Model Fitting 1061
20.4.9 Spectrum Stripping 1067
20.4.10 Library Least-Squares 1068
20.4.11 Symbolic Monte Carlo 1070
20.5 Radiation Spectroscopy Measurements 1071
20.5.1 Channel Calibration 1071
20.5.2 Quality Metrics 1072
20.5.3 Detection and Spectroscopy with Scintillators 1078
20.5.4 Spectroscopy with Semiconductors 1086
20.6 Factors Affecting Energy Resolution 1088
20.7 Experimental Design 1090
20.7.1 Optimization of Measurement Time 1090
20.7.2 Discernment Between Two Outcomes 1091
20.7.3 Coincidence and Anti-Coincidence Measurements 1094
20.8 Gamma-Ray Spectroscopy—Summary 1102
20.9 Charged-Particle Spectroscopy 1103
20.9.1 Electrons, Positrons, and Beta Particles 1103
20.9.2 Alpha Particles 1106
20.9.3 Heavy Ions 1109

21 Mitigating Background 1119


21.1 Sources of Background Radiation 1120
21.1.1 Cosmic Radiation 1120
21.1.2 Natural Occurring Radioactivity 1124
Contents xix

21.1.3 Airborne Radioactivity 1132


21.1.4 Modern Radiation Sources 1133
21.2 Mitigation of the Radiation Background 1133
21.2.1 Sample Placement 1136
21.2.2 Minimize Radioactivity in the Detector System 1136
21.2.3 Passive Shielding of Radiation Spectrometers 1138
21.2.4 Shielding Against Gamma Rays 1139
21.2.5 Shielding Against Neutrons 1142
21.2.6 Minimize Radioactivity in Air around Spectrometer 1142
21.2.7 Use Construction materials with Low Radioactivity 1143
21.2.8 Counting Enclosures 1143
21.2.9 Laboratory Location 1144
21.2.10 Other Considerations 1145
21.3 Self-Absorption of Photons 1147
21.3.1 Infinite Slab 1147
21.3.2 Infinite Cylinder 1149
21.4 Electronic Methods for Background Reduction 1150
21.4.1 Anti-coincident Background Reduction 1151
21.4.2 Coincident Counting 1151

22 Nuclear Electronics 1155


22.1 Mathematical Transforms 1155
22.1.1 The Fourier Transform 1156
22.1.2 The Laplace Transform 1156
22.1.3 Properties of the Laplace Transform 1158
22.1.4 The Transfer Function 1160
22.2 Pulse Shaping 1161
22.2.1 Circuit Element Impedances 1162
22.2.2 Operational Amplifier 1165
22.2.3 The General Case for Feedback Transfer Function 1166
22.2.4 Passive Low-Pass Filter 1166
22.2.5 Active Low-Pass Filter 1168
22.2.6 Passive High-Pass Filter 1169
22.2.7 Active High-Pass Filter 1175
22.2.8 CR-RC Network 1176
22.2.9 (CR)2 -RC Network 1178
22.2.10 CR-(RC)n Network 1178
22.2.11 Delay Line Pulse Shaping 1179
22.2.12 Pole-Zero Cancellation 1180
22.2.13 Base-Line Shift and Restoration 1181
22.3 Components 1182
22.3.1 Preamplifiers 1182
22.3.2 Amplifiers 1189
22.3.3 Integral Discriminators and Single Channel Analyzers 1195
22.3.4 Counters (Scalers) and Timers 1197
22.3.5 Ratemeter 1198
22.3.6 Multichannel Analyzers 1200
xx Contents

22.3.7 Pulse Generators 1203


22.3.8 Power Supplies 1204
22.4 Timing 1205
22.4.1 Jitter and Time Walk 1205
22.4.2 Common Timing Methods 1206
22.5 Coincidence and Anti-Coincidence 1208
22.5.1 Coincidence Analyzers 1209
22.5.2 Time-to-Amplitude Converter 1212
22.6 Instrumentation Standards 1214
22.6.1 NIM Standard 1214
22.6.2 CAMAC Standard 1217
22.6.3 VMEbus Standard 1221
22.7 Electronic Noise 1223
22.7.1 Thermal or Johnson Noise 1225
22.7.2 Shot Noise 1226
22.7.3 Flicker or 1/f Noise 1226
22.7.4 Detector Performance 1227
22.8 Coaxial Cables 1230
22.8.1 Basic Characteristics 1231

A Fundamental Physical Data and Conversion Factors 1241


A.1 Fundamental Physical Constants 1241
A.2 The Periodic Table 1242
A.3 Physical Properties and Abundances of Elements 1242
A.4 SI Units 1243
A.5 Internet Data Sources 1243

B Cross Sections and Related Data 1249


B.1 Data Tables 1249
B.1.1 Thermal Neutron Interactions 1249
B.1.2 Photon Interactions 1250

Index 1269
Preface

Ever since the discovery of x rays by Röntgen almost 125 years ago, who used fluorescing barium-
platinocyanide coated plates and later photographic film as the first radiation detectors, there has been
increasing activity in the design and development of detectors to measure ionizing radiation. Early radiation
detector development was driven by both the discovery of new types of ionizing radiation and a better under-
standing of how radiation interacts with matter. In the last half of the twentieth century detector technology
saw major advances with the introduction of supporting electronics, notably the photomultiplier tube, and
the introduction of new detector materials such as semiconductors and new scintillator materials. In this
era, the fundamental principles of radiation detection and measurement were firmly established. Then in the
last two decades, a vast number of researchers introduced an ever increasing number of new detector designs,
almost all based on twentieth century technology. In the past decade the introduction of new variations in
basic detector technology has become a growth industry, fueled largely by national security concerns and
government sponsorship.
At the same time that radiation detector technology was advancing, many books on the subject were
introduced. Many were limited to a single aspect or type of detector technology and were intended for
a specialist in radiation detection and, consequently, were not suitable as texts in courses on radiation
technology. Other books designed primarily as text books attempted to present a broad coverage of the
many facets of radiation detections but were somewhat superficial because of their reliance on old analyses,
rules of thumb, simple derivations, and a limited number of detector designs. Yet other more ambitious
text books became encyclopedic by trying to cover the many different types of detectors while necessarily
scrimping on analytic details or simply quoting analytical results. Also lacking in most of these treatises was
a review of the history of radiation detector development and a presentation of the important milestones
achieved by the vast research on radiation detection.
When we embarked on this book project over ten years ago, we envisioned a book that could serve both
as a text for different courses in radiation detection and as a reference work for practitioners in radiation
detection. Four goals guided us: (1) to include information about the historical development and the major
achievements in detector technology, (2) to provide fundamental information about radiation interactions,
nuclear physics, and electrostatics, (3) to present a broad and detailed coverage of the many types of radiation
detectors that have been introduced, and (4) to present important mathematical models and analyses used in
detector designs and applications. With these goals in mind, we have attempted to develop the fundamentals
of radiation detection and detector technology so that a researcher or user of these devices can understand
radiation interactions in materials, physics of the radiation detectors, commercially available and conceptual
detectors, detector designs, characterization techniques, and special electronics used for various detector
configurations and applications. Many of the topics covered are interrelated and, hence, the presentation of

xxi
xxii Preface

these topics could be arranged in a number of different ways. The sequence chosen by us was done so as to
reduce redundancy while, at the same time, to develop a logical and clear path of presentation.
Overall, this book is designed to give the reader more than a glimpse at radiation detection devices and
a few packaged equations. Rather it seeks to provide an understanding that allows the reader to choose
the appropriate detection technology for a particular application, to design detectors, and to competently
perform radiation measurements. For this reason, there are many equations derived from first principles,
derivations which may seem tedious to some readers. Yet, we believe that a firm understanding of the
assumptions used to derive many frequently encountered equations used in the discipline helps a radiation
detector user to decide when, and also when not, to apply them, and how to arrive at an appropriate
alternative, if needed. Many of the later chapters on specific aspects of radiation detectors attempt to
provide a comprehensive review of the historical development and current state of the topic. Such a review
necessarily entails citations to many of the important discoveries and the many references provided allow a
reader to quickly find additional and more detailed information.
This book has five main themes: General Concepts for Radiation Detection, Common Radiation Detector
Properties, Types of Radiation Detectors, Radiation Measurements, and finally a single chapter on Intro-
ductory Electronics. Although these themes are represented by various chapters, there is some redundancy
between chapters both because the themes are closely related and because some overlap assists with clarity.
For instance, semiconductor photodiodes are used as light collecting devices for some scintillators, hence
there is a discussion on photodiodes in the chapter on light collecting devices. Yet, the physics of semicon-
ductor diode detectors is detailed in those chapters covering semiconductor detectors, which comes after the
chapter on light collecting devices. This order may seem out of sequence, yet is unavoidable because the
chapters on scintillator detectors precede the chapters on semiconductor detectors, and the authors deem
it best to include the chapter on light gathering devices next to the chapters on the scintillation detectors
because they are used together as a single unit. Neutron detectors are configured as gas-filled, scintillator,
and semiconductor devices, as well as a few special detector designs. As a result, there are chapters dedicated
specifically to neutron detectors. Yet many of the principles of these neutron detectors borrow heavily from
those concepts outlined in the chapters dedicated to gas-filled, scintillator, and semiconductor detectors.

Acknowledgments
Although we have included a few original contributions, the vast amount of material presented is the result
of the work by thousands of researchers in radiation detection and its related fields. For their efforts and
for what they have taught us we are extremely grateful. Although it is impossible to give credit to all of
these specialists, we have attempted to cite many of the key papers, reports and books that have guided the
development of radiation technology. Because of the breadth of the goals for this book, the time required to
write it and its resulting size are unusually long. Special thanks go our publisher’s forbearance and patience
in this book project.
The authors acknowledge and give their appreciation for the support and assistance of numerous indi-
viduals who made this project possible through their contributions, guidance, and encouragement. Great
appreciation is extended to those current and former students who took time to proofread this text and, in do-
ing so, made valuable contributions and suggestions. These include Elsa Ariesanti, Steven Bellinger, Brian
Cooper, Benjamin Damm, Nathaniel Edwards, Ryan Fronk, Priyarshini Ghosh, Nikolas Hinson, Alireza
Kargar, Michael Meier, Benjamin Montag, Kyle Nelson, Taylor Ochs, and Michael Reichenberger. Many
of these same students contributed to text material in the form of radiation detection data and instrument
photographs. We thank the library staff at Kansas State University for acquiring the several hundreds of
citations, many rare and difficult to locate, used in the references listed at the end of each chapter. Special
gratitude is extended to Rick Brake (retired Los Alamos Nat. Lab.), Anthony Caruso (UMKC), Stephan
Friedrich (LLNL), Kimberlee Kearfott (U. Michigan), Mike Kusner (Saint-Gobain), Michael Mayhugh (re-
Preface xxiii

tired Saint-Gobain), Tim Sobering (KSU), and Jack Thiesen (U. Michigan) for reviewing certain chapters
of this book and providing valuable comments, corrections, and improvements.
The authors also extend appreciation to their colleagues and friends who contributed to the knowledge
and material presented in the text. These include Anthony Caruso (UMKC), Elias Chavez (Ludlum), Paul
Davison (ADIT), William Dunn (Kansas State U.), Peggy Groff (Photonis), Daniel Herr (Saint-Gobain
Crystals), Kimberly Kearfott (U. Michigan), Ben Kennedy (Ortec Ametek-AMT), Mike Kusner (Saint-
Gobain Crystals), Bill Lehnert (LND, Inc.), Michael Mayhugh (retired Saint-Gobain Crystals), Jeremy
Roberts (Kansas State U.), Ronald Rojeski, and Ron Stubberfield (ET Enterprises).
A special acknowledgement is extended to Richard (Rick) Brake, whose encouragement and financial
support allowed one author (McGregor) to build his first radiation detectors while a graduate student intern
at Los Alamos National Laboratory. Along with Rick Brake were those who took time to teach the author
fundamentals of semiconductor device fabrication and detector construction, including Victor Swenson and
Bill Gibler of Texas A&M University, and Alan Gibbs and David Brown of Los Alamos National Laboratory.
It is the initial encouragement from these mentors that eventually led to the compilation of this text. Also
acknowledged is former advisor and instructor Mark Weichold of Texas A&M University, whose constructive
and detailed explanations of solid state and semiconductor physics have served one author (McGregor) well.
Above all we have valued the support and encouragement of our wives, Vilelmina and Sue, whose for-
bearance of too many evenings of neglect because of this tome will forever be remembered and appreciated.
Manhattan, Kansas Douglas S. McGregor
June 2019 J. Kenneth Shultis
About the Authors

Douglas S. McGregor, born in Dallas, Texas in 1957, received BA (1985) and MS (1989) degrees, both in
electrical engineering, at Texas A&M University. He then received MS (1992) and PhD (1993) degrees, both
in nuclear engineering, from the University of Michigan. From 1994 to 1996 he held a post doctoral position
at Sandia National Laboratory in Livermore, California before returning to the University of Michigan where
he was an assistant research professor from 1997 to 2002. In 2002, he joined the Nuclear Engineering faculty
at Kansas State University (KSU) where he now is a University Distinguished Professor and holds the
Boyd D. Brainard Chair in Mechanical and Nuclear Engineering. Professor McGregor serves as director
of the Semiconductor Materials and Radiological Technologies Laboratory at KSU, a 9500 sq ft laboratory
dedicated to radiation detector research.
Professor McGregor teaches and conducts research on the design, development, and deployment of ra-
diation detectors and detector systems. In particular, he develops systems for measuring various ionizing
and non-ionizing radiations based on semiconductor, scintillator, and gas-filled detectors. He specializes in
semiconductor device physics, semiconductor device designs, radiation detector physics, neutron detector
designs, and radiation detection and measurement. He has published over 200 research articles and reports,
is co-inventor on over 20 radiation detector patents, and his research group has received five R&D-100
Awards for radiation detector innovations. Prof. McGregor is also the recipient of various other honors,
including the KSU College of Engineering (CoE) Frankenhoff Outstanding Research Award (2006) and the
CoE Engineering Distinguished Researcher Award (2016).

J. Kenneth Shultis, born in Toronto Canada in 1941, graduated from the University of Toronto with a
BASc degree in Engineering Physics. He gained his MS (1965) and PhD (1968) degrees in Nuclear Science
and Engineering from the University of Michigan. After a postdoctoral year at the Mathematics Institute
of the University of Groningen, the Netherlands, he joined the Nuclear Engineering faculty at Kansas State
University in 1969 and where he presently holds the Black and Veatch Distinguished Professorship and is
the Ike and Letty Conerstone teaching scholar.
Professor Shultis teaches and conducts research in neutron and radiation transport, radiation shielding,
reactor physics, numerical analysis, particle combustion, remote sensing, and utility energy and economic
analyses. He has had a rich collaboration in research and scholarship. Besides being coauthor of this
book he has coauthored the books Fundamentals of Nuclear Science and Engineering, Radiation Shielding,
Radiological Assessment, Principles of Radiation Shielding, and Exploring Monte Carlo Methods. In addition,
he has produced over 150 research papers and reports and served as a consultant to many private and
governmental organizations. He is a Fellow of the American Nuclear Society (ANS), and has received many
awards for his teaching and research, including the infrequently awarded ANS Rockwell Lifetime Achievement
Award for his contributions over 50 years to the practice of radiation shielding.

xxv
Chapter 1

Origins

Great discoveries are made accidentally less often


than the populace likes to think.
Wilhelm Röntgen

1.1 A Brief History of Radiation Discovery


In 1895, within the town of Strasbourg (then located in Germany, but
now in France), Wilhelm Conrad Röntgen (see Fig. 1.1) made the first
observation of mysterious penetrating rays. For many years, these myste-
rious rays were called “Röntgen rays”; however, Röntgen actually named
them “x rays,” as we know them today, after the common algebraic sym-
bol for an unknown. In the famous experiment, Röntgen was operating
a type of Crookes tube (see Fig. 1.2) while performing experiments with
“cathode rays.” With the Crookes tube covered with black paper, he
noticed that a plate coated with barium-platinocyanide (BaPt(CN)4 ),
located approximately six feet away in the darkened room, was glowing.
By placing objects with varying densities and thicknesses between the
Crookes tube and the plate, he deduced that the mysterious emanations
originated from the Crookes tube and that they were attenuated accord-
ing to mass density and thickness of the absorber. A short while later,
it was discovered that x rays are actually a form of electromagnetic radi-
ation emitted from accelerated charged particles (electrons in Röntgen’s
experiment). Röntgen also used photographic plates for his studies after
he learned that film emulsions were exposed by the x rays. After experi-
menting with many x-ray image exposures of inanimate objects, perhaps
the most famous x-ray photograph he developed is traditionally believed Figure 1.1. Wilhelm Conrad Röntgen
to be an image of his wife’s hand, Bertha Röntgen (see Fig. 1.3). Indeed (1845–1923).
photographic film is a type of radiation detector, and the x-ray image
of Bertha Röntgen’s hand marks the beginning of medical imaging. For his discovery of x rays, Röntgen
became the recipient in 1901 of the first Nobel Prize in Physics. These discoveries were made with two types
of radiation detectors, namely the scintillating BaPt(CN)4 -coated plate and the photographic plates.
In 1896, shortly after the announcement of the discovery of x rays, Henri Becquerel (Fig. 1.4), while
conducting experiments with his father’s geology samples, discovered natural radiation emissions. It was
already known that many substances could be made to fluoresce by exposing them to visible light, and
Becquerel was studying the fluorescence of sulphates of uranium and potassium by exposing his samples

1
2 Origins Chap. 1

Figure 1.2. A Crookes tube was used as the x-ray source in Röntgen’s ex-
periments. The Maltese cross in the vacuum tube is connected to a hinge that
allows it to be flipped up or down.

Figure 1.3. (Left) Traditionally labeled as Bertha Röntgen’s hand, and probably
the case, it actually was not labeled as such at the time of publication. (Right)
Often mistakenly labeled as Bertha Röntgen’s hand, this image taken by Röntgen is
actually that of Alfred von Kölliker’s hand. The discovery that x rays can be used
to produce images of bone structure marks the beginning of the modern medical
imaging profession.
Sec. 1.1. A Brief History of Radiation Discovery 3

Figure 1.4. Antoine Henri Bec- Figure 1.5. The original photographic plate images,
querel (1852–1908). taken by Henri Becquerel, of uranium ore samples.

to sunlight and measuring the light emissions with photographic plates. In one instance, he prepared a
sample set of uranium salts for an exposure experiment, but decided to delay the experiment that day due
to cloudy weather. Instead, he placed the uranium salt samples in a dresser drawer, fortuitously atop a stack
of photographic plates. A few days later, he decided to check the quality of his photographic plates before
trying the fluorescence experiment again, and developed the top photographic plate on which the samples
lay, only to find that an image had formed (see Fig. 1.5). At first, Becquerel actually thought that the
uranium salt samples were exposed to enough light to cause fluorescence, which he believed then exposed
the film. He continued to conduct the experiments, but instead covered the photographic plates with black
paper, upon which he placed the samples. He later discovered uranium salts not yet exposed to sunlight had
the same effect on the photographic plates. Finally, several months after the initial discovery, he found that
non-fluorescent uranium ore could also expose the plates, and he deduced that unknown emanations from
the rock samples themselves caused the exposure. Initially referred to as “Becquerel rays,” we now know
the emanations he observed were a combination of alpha particles, beta particles, and gamma rays. For the
discovery of radioactivity, Becquerel shared in the third Nobel Prize in Physics in 19031 along with Pierre
and Marie Curie for their work and discovery of polonium and radium. Again, the discovery was made
possible with a type of radiation detector (photographic plates). It is interesting to note that in February
1896 an English physicist and mathematician by the name of Silvanus Thompson independently conducted
the same experiment as Becquerel, in which he exposed uranium samples to sunlight as they were placed
upon a paper-covered photographic plate. He also discovered the mysterious emanations, but when he sent
his results in for publication (to the Royal Society in London), he was informed that Becquerel had already
reported the same findings only two weeks earlier to the French Academy of Sciences.
During the 1890s, many other significant experiments were being conducted with cathode ray
tubes. Cathode ray tubes were built in many configurations, but common features included a neg-
atively charged electrode (cathode) and a positively charged electrode (anode) sealed in an elon-
gated vacuum tube, where the far end of the tube opposite the cathode was coated with a phosphor.

1 Interestinglyenough, there is evidence that natural radiation had been observed from uranium salts much earlier by Claude
Félix Abel Niepce de Saint-Victor, in which a uranyl nitrate sample had been brought into close proximity to a photo sensitive
paper sheet [Saint-Victor 1858]. The Niepce de Saint-Victor experiments were reported to the French Academy of Sciences
in 1858, and evidently Becquerel was aware of the work [Fournier and Fournier 1990]. Regardless, Becquerel was the first to
explain and understand the significance of the discovery.
4 Origins Chap. 1

_ phosphor
+ coating
+ deflection
anode plug electrodes
cathode

slits scale to measure


_ evacuated ray deflection
glass vessel

Figure 1.7. The cathode ray tube apparatus used by Thomson to measure the q/m
ratio for cathode rays.

In 1895, through the use of a cathode ray tube, Jean Baptiste Perrin made the discovery that
cathode rays were composed of negative electricity. Building on this knowledge, Joseph John
Thomson (see Fig. 1.6) conducted experiments with different cathode
ray tubes (CRTs) to investigate the nature of the cathode rays, where
he paid special attention to evacuating the CRT. This simple precaution
allowed experiments to be conducted without contaminant gases which
could become ionized during the operation of the tube. A schematic of
such a tube is shown in Fig. 1.7. With these tubes Thomson made
three fundamental experimental observations. First, he noted that
magnetic fields and electric fields could deflect the trajectory of the
cathode rays.
Further, given a known magnetic field strength, he noted that the
deflection of these cathode rays was far greater than observed for pos-
itively charged hydrogen gas. Finally, by comparing the results of the
cathode rays and the hydrogen gas, Thomson noted that the charge-
to-mass ratio was approximately 1800 times greater for the cathode
rays than for hydrogen ions.2 Because he was confident no gas was
inside the cathode ray tube, in 1897 Thomson correctly deduced that
cathode rays were in fact negatively charged particles emitted from the
cathode surface or, more correctly, emitted from the atoms composing Figure 1.6. Joseph John Thomson
the cathode. Although Thomson named these newly identified nega- (1856–1940).
tive particles “corpuscles,” the eventual name given to them was electrons as suggested by George Johnston
Stoney, who had actually predicted the presence of these negative particles as early as 1874.
It should be noted that Thomson’s discovery was the first recorded indication that atoms consisted of
subatomic particles, thereby, earning him the 1906 Nobel Prize in Physics. Thomson’s discovery was made
possible, in part, with another type of radiation detector, namely the fluorescent screen of the CRT.
The observations and findings of Becquerel caught the interests of Pierre and Marie Curie, both chemists
by education (see Fig. 1.8). Marie began studying under Becquerel, and began a systematic investigation
of the known elements to determine if other materials emitted energetic rays similar to those from ura-
nium. While studying pitchblende, an uranium ore containing various oxides, thorium, and other rare earth
elements, she found that thorium and thorium compounds also emitted energetic rays. Marie is generally

2 Thesame observation was made by Arthur Schuster in 1890, where he also measured the charge-to-mass ratio of cathode rays
to be over 1000 times greater than positively charged hydrogen gas. However, he believed the measurements to be in error
and his observations went largely unnoticed.
Sec. 1.1. A Brief History of Radiation Discovery 5

credited with recommending the name radioactivity 3 to describe


these energetic emissions. Marie quickly reported these findings,
only to learn that German physicist Gerhard Schmidt had published
similar findings on thorium only two months earlier. However, of
genuine interest in Curie’s work was the observation that the pitch-
blende, after removing the uranium, was more radioactive than the
uranium. The Curies thus deduced correctly that another radioac-
tive element must be present.
In 1898, Pierre joined Marie’s research effort, and together they
worked to separate and identify the other radioactive substances in
pitchblende. They used a quartz piezoelectric electrometer (named
a Curie electrometer), invented by Pierre and his brother Jacques, to
measure the ionization produced in air by the radiation emitted from
the purified samples. They separated literally tons of pitchblende
material to attain just a few milligrams of the purified radioactive
substance, which they named polonium (after Marie’s country of
birth, Poland) and they reported the new material in July 1898.
Five months later in December 1898, they reported a second new
element, which they named radium. For their work on radioactive
materials, both Pierre and Marie Curie shared the 1903 Nobel Prize Figure 1.8. Marie (1867–1934) and
Pierre (1859–1906) Curie discovered polo-
in Physics with Henri Becquerel. Marie Curie also received the 1911 nium and radium.
Nobel Prize in Chemistry for discovering two new elements4 (Pierre
had been accidentally killed by a horse and wagon in 1906, and did not share in the award).
In 1899 Ernest Rutherford (see Fig. 1.9), who was a former student of J.J. Thomson, took on the task
of identifying the natural radiation discovered by Becquerel. Rutherford used a gold foil electroscope as
the detector in his experiments. Understanding that the radiation pro-
duced free charges in air, he placed a uranium ore sample in the elec-
troscope compartment, charged the electroscope, and then recorded the
discharge rate of the gold foils. Rutherford then placed thin layers of alu-
minum foil (each 5-μm thick), one at a time, over the uranium ore sample.
For each foil added, he observed the change in the discharge rate. He noted
that a significant change in discharge rate occurred each time for the first
three foils used, but the change in discharge rate was dramatically less
afterwards. In fact, after the first three foils were in place the discharge
rate had dropped to 8% of the initial rate with no attenuators. However, it
took an extra 100 aluminum foil layers to reduce the discharge rate to 2%
of the initial rate. Rutherford correctly deduced that two types of radia-
tion were present. He named those radiations stopped with only three foils
alpha rays and those higher penetrating radiations were named beta rays.
We now know these rays to be particles, with α particles being 4 He nuclei
and β particles being electrons. For these discoveries, Ernest Rutherford
Figure 1.9. Sir Ernest Rutherford
was awarded the 1906 Nobel Prize in Chemistry. Using magnetic fields, (1871–1937) discovered alpha and
Rutherford later showed that beta particles could be easily deflected, while beta particles.

3 The word radioactivity was chosen because of its Latin root word “radius,” which means ‘ray’ or ‘spoke of a wheel.’
4 Marie Curie is the first (and presently only) person to receive Nobel prizes in two different scientific fields.
6 Origins Chap. 1

Figure 1.10. Paul Ulrich Villard Figure 1.11. Arthur Holly Compton (1892–
(1860–1934) discovered what were later 1962) discovered what is known as Compton
called gamma rays. scattering.

alpha particles were deflected very little, and in the opposite direction of beta particles, indicating different
masses and different characteristic charges.
Shortly thereafter, in 1900, Paul Villard (see Fig. 1.10) conducted experiments with radium samples and
photographic plates. He collimated the radiation from a radium sample towards a photographic plate that
was shielded with a thin layer of lead. The lead stopped the α particles, but allowed the highly penetrating
radiation to pass. Using a magnetic field, he noted that two types of penetrating radiation were present,
one type that was deflected by a magnetic field, and another that was not. He concluded that the deflected
radiation was composed of the β particles discovered by Rutherford, but the undeflected radiation must be
a third and different kind. Initially, Rutherford thought these emanations to be nothing more than highly
energetic β particles, but eventually came to believe that Villard was correct. Villard did not name the
radiation he discovered, but instead, in 1903, it was Rutherford who named the third radiation gamma rays.
In 1914 it was shown that these highly penetrating rays, which were not affected by magnetic fields, could
also be diffracted off crystal surfaces. Hence, Villard was correct, and gamma radiation was something quite
different. The nature of gamma rays was explored further in 1918 by Arthur Holly Compton (see Fig. 1.11),
who developed the fundamental physics behind what is referred to as Compton scattering. He showed that
gamma rays lose energy after scattering with electrons, demonstrating the particle nature of gamma rays,
for which he earned the 1927 Nobel Prize in Physics.
Noted in Millikan’s book Electricity, Sound and Light [1908], there were certain aspects of the atom
not clearly understood. For instance, as Millikan deduced, because electrons possess negative electricity and
atoms themselves are neutral, then there must be some form of positive charge within the atomic structure to
cancel the negative charge of the electron. J.J. Thomson proposed an atomic model, later disproved, in which
the atomic nucleus consisted of positive electricity (now known as protons) about which, or within which,
the negative electrons were rotating. This model is often referred to as the “plum pudding model,” with
the pudding being the positive stuff and the electrons the plums. In 1909, Ernest Rutherford performed an
important experiment that proved the plum pudding model wrong. In his experiment, Rutherford collimated
Sec. 1.1. A Brief History of Radiation Discovery 7

Figure 1.12. Charles Thomson Rees Figure 1.13. Robert Andrews Mil-
Wilson (1869–1959). likan (1868–1953).

alpha particles from a Po sample into an ultra-thin sheet of Au foil, using the alpha particles as a method to
probe the atomic structure of Au. If Thomson was correct and the Au atoms resembled the plum pudding
model, then the alpha particles should just pass through the Au foil with hardly any deflection. Although
Rutherford found that many alpha particles did actually pass directly through the Au foil, he also found
that a small fraction were strongly deflected, and some scattered in the backwards direction. He concluded
that such strong interactions could only happen if the positively charged alpha particles came into the
close vicinity of another small but heavy positive mass, unlike the small deflections expected from the large
neutralized atomic core suggested by Thomson. From his findings, Rutherford postulated the following:
(1) Most of the atomic mass and positive charge are contained in a small core called the nucleus.5
(2) Most of the volume of the atom is empty space about which the negative electrons are dispersed.
(3) Within the atom, the number of negatively charged electrons and the number of positively charged
particles (protons) are equal.
In 1911 Charles Wilson (see Fig. 1.12) devised what is now known as a cloud chamber6 to visualize the
paths of charged particles by trails of condensed droplets in supersaturated water vapor and air mixture.
These vapor trails would drift downwards under the influence of gravity. Wilson realized that the ion trails
could be forced downwards faster by applying an electric field such that the droplets fell under the influence
of both gravity and the electrostatic field [Kaplan 1962]. Wilson managed to obtain an estimate of the charge
of an electron by comparing the rates of fall with and without the electric field force applied. However, two
significant errors prevented accuracy, namely (a) the droplets could reach terminal velocity in the air and
water vapor mixture regardless of the applied field, hence a true measure of the electric field influence was
not possible, and (b) a water droplet would begin to evaporate so that the droplet mass changed as the cloud

5 Traditionally,because of his identification of a distinct positive core within the atom, Rutherford is credited with discovering
the proton.
6 Wilson received the 1919 Nobel Prize in Physics for this interesting detection device.
8 Origins Chap. 1

trail fell downwards. Further, Wilson measured only the upper part of the cloud trails because the lower
droplets in the trails were more heavily charged and generally moved faster than the upper portion.
Robert Millikan (see Fig. 1.13) thought that Wilson’s method could be improved by applying the electric
field force in the opposite direction of gravity so that the tiny charged vapor droplets could be made to remain
stationary (balancing electric field and gravitational forces). No assumptions need be made about terminal
velocities and what portion of the cloud should be inspected. Specific droplets could be selected, using a
microscope, and observed. However, the problem remained that water and alcohols quickly evaporated. As
the story goes, Millikan thought of the idea of substituting clock oil for water vapor while on a train trip.
When looking at his watch, he realized that clock oil was used as a long lasting lubrication because it did
not evaporate. Using an atomizer to inject a fine mist of oil droplets into a chamber, Millikan irradiated
the chamber with x rays to produce charges on the oil droplets (see Fig. 1.14). He held a single droplet
stationary by balancing the electric field force with the gravitational force. Regardless of the droplet chosen,
he observed that the measured electric field (coulombs per unit distance) required to hold an oil droplet
stationary were multiples of 1.6 × 10−19 coulombs. A single oil droplet might have an excess or deficiency
of one or more electrons, but could not gain or lose a fraction of an electron.7 This measurement also led to
the electron mass being estimated as 9.1 × 10−31 kg, again remarkably close to the presently accepted value
of 9.109 382 91 × 10−31 kg.

metal chamber

oil atomizer

small hole
in electrode

+
microscope _

planar +
x-rays electrodes
_
Figure 1.14. The basic components of Millikan’s oil drop apparatus.

In 1920, Rutherford noted that there was some problem balancing the atomic masses of elements and
their charge. For instance, the mass of hydrogen could be measured, as could other elements. It had also

7 There is controversy over Millikan’s selective use of data, in which over 60% of his recorded measurements were not included in
his publications. Note also that a great controversy arose between Millikan and Felix Ehrenhaft, who also tried to measure the
fundamental negative charge. Ehrenhaft’s data suggests the existence of a smaller fundamental charge, sometimes recorded as
low as 1/10 that of 1.6 × 10−19 coulombs. It has been suggested that Ehrenhaft may have observed the effect of elementary
particles (such as quarks), although a more likely explanation is that the observed differences were a result of experimental
error. Regardless, Millikan’s conclusion, reported in 1913, has less than 0.5% error of the presently accepted value of qe =
1.602 176 565 × 10−19 coulombs. Delayed by the “Millikan-Ehrenhaft controversy,” Millikan did eventually receive the Nobel
Prize in Physics (1923) for his work.
Sec. 1.1. A Brief History of Radiation Discovery 9

been determined that a proton had an intrinsic charge equal in magnitude to that of an electron, yet opposite
in polarity. This all made sense, except that the masses did not scale linearly with the quantity of electrons
or protons. Rutherford hypothesized, therefore, that some additional mass, neutral in nature, must be
present. Many years later, in 1928, experiments were conducted by Walther Bothe8 and Herbert Becker
where alpha particles from Po were used to bombard Be. The result was the discovery of a new form of
highly penetrating neutral radiation. Initially thought to be high energy gamma rays, this idea was quickly
discarded as unlikely because of the constraints of conservation of energy and mass requirements in Compton
scattering. Irene Curie (daughter of Marie and Pierre Curie) and her husband, Frédérick Joliot, studied the
effects further by also bombarding Be with alpha particles emitted from Po, causing the unidentified neutral
radiation to be emitted into a paraffin sample. The result was the emission from the paraffin of energetic
protons. These protons were measured with a gas-filled counter (a detector developed by Hans Geiger and
Ernest Rutherford) to have approximately 5.3 MeV of kinetic energy. From Compton’s previous findings
with gamma-ray scattering, the observed result was unlikely if the unknown neutral emissions really were
gamma rays.
James Chadwick (see Fig. 1.15), who was Rutherford’s student, used a similar arrangement as
Curie and Joliot with a few changes. A Po alpha particle source was used to produce the neutral
particles from a boron sample, and a gas-filled detector similar to early Geiger models was placed
near the Be sample such that the neutral emissions could enter the detector [Chadwick 1932]. Sep-
arately using N2 and then H2 gas in the detector, along with conservation of mass and energy cal-
culations, Chadwick measured and calculated the mass (or energy) of the neutral radiation to be
938 MeV/c2 , nearly the same, but slightly larger than that of protons. Thus, Chadwick found
the missing particle that Rutherford had hypothesized, and because they have no intrinsic charge,
he named them neutrons. Remarkably, Chadwick’s calculations were
within 0.17% error of the presently accepted value of 939.272 046
MeV/c2 . For the discovery of neutrons, Chadwick received the 1935
Nobel Prize in Physics.
Following the discovery of these basic subatomic particles (electrons,
protons, and neutrons), numerous other subatomic particles and ele-
mentary particles have been discovered. Quarks are elementary parti-
cles that combine to form hadrons, and all quarks follow Fermi-Dirac
statistical models in which no quark can occupy the same quantum state
as another. Hence, quarks belong to the group of particles classified as
fermions. Independently postulated as existing by Murray Gell-Mann
and George Zweig in 1964, the quark was discovered in 1968 at the
Stanford Linear Accelerator Center (SLAC). Gell-Mann received the
1969 Nobel Prize in Physics for his contributions to the theory and his
prediction of the quark.
There are six types of quarks, with the fanciful names of up, down,
top, bottom, charm and strange, in what is now known as the stan-
Figure 1.15. James Chadwick (1891– dard model. Hadrons are subcategorized as mesons and baryons, where
1974) discovered neutrons.
mesons are composed of two quarks and baryons are composed of three
quarks. The two most well-known and stable baryons are protons and neutrons. Protons are composed
of two up-quarks (each with charge of +2/3 qe ) and one down-quark (charge of −1/3 qe), yielding a total

8 Walther Bolthe used Geiger counters to invent a method of coincidence counting in 1924. He used this technique to discover
and verify several physical principles about penetrating radiation and light quanta. For his invention of coincidence counting,
and his many discoveries, he received the 1954 Nobel Prize in Physics.
10 Origins Chap. 1

charge of +qe . Neutrons are composed of one up-quark and two down-quarks, yielding a total neutral charge.
Neutrons not bound in an atomic nucleus are radioactively unstable with a half-life of 10.23 minutes. When
a neutron is free from an atomic nucleus, one of the down-quarks decays into an up-quark, causing the
neutron to decay into a proton, an electron, and an antineutrino.
The existence of mesons, a particle with binding force capable of holding the atomic nucleus together,
was predicted by Hideki Yukawa in 1935. Convincing evidence of Yukawa’s theory was found in 1945 with
the discovery of the π-meson (pion) at the University of Bristol, a particle that was later proved to have a
strong nuclear force that participates in binding of the nucleus. Yakawa received the 1948 Nobel Prize in
Physics for his theory on the behavior and properties of mesons, in particular, the pion.
Another set of elementary particles are the leptons, also classified as fermions, which are categorized into
six flavors subdivided as three generations. The electronic generation is composed of electrons and electron-
neutrinos, the second generation is composed of muons and muon-neutrinos, and the third generation is
composed of tauons and tauon-neutrinos. The existence of the various neutrino forms was discovered in
1962 by Leon M. Lederman, Melvin Schwartz, and Jack Steinberger who were awarded the 1988 Nobel Prize
in Physics.
All fermions (hadrons and leptons) have corresponding anti-particles. For hadrons the anti-particle is
composed of the corresponding anti-quarks producing anti-hadrons with identical mass but opposite charge
as their real hadron counterparts. In fact anti-matter seems to interact with the strong and electromagnetic
forces identically as does matter. Thus, it is possible to envision anti-atoms and macroscopic masses composed
of anti-matter. However, matter and anti-matter cannot coexist. Just as positrons annihilate with electrons,
anti-nucleons annihilate with nucleons.
Finally, a third branch of elementary particles contains the bosons consisting of photons, gluons, Z and
W± particles. These particles are governed by Bose-Einstein statistics and, hence, they can occupy the
same quantum state at the same time. Photons represent the force component of an electromagnetic field,
gluons are the strong binding force among the quarks in the neutron and proton as well as the binding of
the nucleons in an atomic nucleus, and the Z and W± particles are responsible for the so-called weak nuclear
force. A fifth boson, the Higgs boson (H0 ) is a theoretical particle predicted by the standard model, but for
years it remained elusive. Finally in 2012, researchers at the European Organization for Nuclear Research
(known as CERN) announced its discovery, completing the search for all the elementary particles required
by the standard model. This last boson is important because it is the particle that gives mass to all the
other elementary particles.
Today the search for a better understanding of the sub-atomic realm continues. The ingenious methods
used by Thompson, Rutherford, Millikan and their contemporaries have been largely replaced with enormous
particle accelerators and sophisticated detection systems. Rather than a single observer performing experi-
ments in a one-room laboratory, teams of physicists and engineers work together at large facilities, such as
CERN, to measure and observe the effects of these numerous elementary particles. Yet, even today, it is the
innovative thought and creativity of individuals that continues to be the driving force behind discovery.

1.2 A Brief History of Radiation Detectors


There are three essential features in any radiation detector. First, the detector must have a material capable
of interacting with the radiation of interest. Otherwise, the radiation would simply pass through it as if no
detector were present. Second, upon interacting with the radiation, the material must exhibit an observable
response. The response can be any of a multitude of possibilities such as temperature changes, color shifts,
light emission, or ionization of the material. Third, the observable must be measurable. For instance,
radiation interactions may occur in a common stone on the ground and ionization may occur in the stone
as a result, but accurate measurement of the ionization is prevented because the stone can not conduct the
Sec. 1.2. A Brief History of Radiation Detectors 11

charges to allow their measurement. A person seeking either to use or to design radiation detectors must
keep these three simple, yet important, concepts in mind.
All the important discoveries of subatomic particles and radiations were accomplished with the use of
various types of radiation detectors, including photographic plates, electroscopes, scintillating materials, and
gas-filled detectors. In the case of photographic film, the absorber is the photo-emulsion, the observable is
the chemical change in the Ag halide crystals in the emulsion, and the measurable is the developable Ag
left behind as an image. In scintillating film, the absorber is the scintillation material, the observable is the
excitation of electrons in the material, which deexcite to give a measurable number of visible photons. In
an electrometer, two Au leaves are held apart by positive charges. When radiation is absorbed in the air
surrounding the Au leaves, it ionizes the air—the observable. Electrons are attracted to the Au leaves and
neutralize some of the charge on the leaves, thereby, causing the Au leaves to move closer together—the
measurable result.
An odd form of radiation detector, not recommended by the authors, is the warming or reddening of
skin from radiation exposure. During the year 1900, Friedrich Walkoff and Friedrich Giesel both conducted
self-exposure experiments with radium. Giesel [1900] reported that he strapped 270 mg of Ra salt to his inner
forearm for hours, and he communicated his observations to Henri Becquerel and Pierre Curie. Walkoff [1900]
reported a similar experiment, except he performed two exposures, each 20 minutes in duration. He wrote
that a skin inflammation formed that had “already lasted over two weeks.” Apparently these findings piqued
the interest of Pierre Curie, who decided to perform a similar experiment of his own [Becquerel and Curie
1901]. He purposely exposed his arm to Ra for several hours, which “resulted into a lesion that resembled
a burn that developed progressively and required several months to heal.” The circumstances surrounding
Becquerel are not as clear, but apparently he carried a glass vial of Ra salts in his vest pocket and developed
a similar radiation burn which took 49 days to heal and left a permanent scar [Becquerel 1903]. In these
experiments the skin tissue was the absorber, the observable was a radiation burn, and the measurable was
the intensity of red as seen by the eye. Amazingly, technicians demonstrating x-ray machines to potential
customers often held one hand near the x-ray tubes until the hand became warm, which indicated to them
that the machine was operating. Since those times, much has been learned regarding the health risks involved
with radiation exposure, and government regulations are in place to limit the radiation dose to civilians and
radiation workers.
As the understanding of radiation interactions in materials increased, more convenient methods of detect-
ing the presence of radiation were sought and developed. For several years after Röntgen’s initial discovery
of x rays, tedious methods were employed using photographic plates, fluorescing screens, or electroscopes.
These early methods of radiation detection relied upon a large amount of radiation exposure and were
not capable of recording individual radiation quanta. The first radiation detector capable of distinguishing
individual radioactive particles was the spinthariscope, invented by Crookes in 1903. It consisted of a ZnS
scintillation screen and a magnifying eyepiece as one unit. Within the device, a tiny Ra source was suspended
by a wire between the eyepiece and the ZnS screen. In a darkened room, the spinthariscope could be used to
visually see individual alpha particle interactions from the radiation source.9 As a post-doctoral researcher
studying under Rutherford, Hans Geiger used the same principle by counting, through a microscope, flashes
of light caused by individual alpha particles as they interacted with a scintillating ZnS screen. The process
was tedious and Geiger would quickly become fatigued.
With the understanding that radiation would ionize gas, in 1908 Ernest Rutherford and Hans Geiger
fashioned a type of gas-filled radiation detector based on the principle of drifting the liberated charges with

9 Believeit or not, spinthariscope rings (named Lone Ranger Atomic Bomb Rings), complete with alpha particle emitting
material, were available from General Mills Cereals between 1947 and the early 1950s for the bargain price of 15 cents and a
Kix cereal box top.
12 Origins Chap. 1

an electric field [Flakus 1981; Frame 2004; Geiger 1913]. This simple detector, at first, consisted of a thin
wire strung coaxially through a metal cylinder. Gas was introduced into the cylinder, and a charged particle
interacting in the gas would produce ionization. The opposite charges (electrons and ions) were drifted
apart by an electric field applied across the wire and cylinder and the charge movement was measured as
a current. The device was redesigned such that the central wire was replaced with a needle point inserted
into a metal cavity, known as Geiger point counters. Later in 1928, returning to the original coaxial design,
Walther Müller (Geiger’s student) improved the device by running the central wire through a glass tube and
attaching the device to electronic tube circuit for readout [Flakus 1981; Frame 2004]. This was an early
version of present day Geiger-Müller counters. Various forms of gas-filled detectors were designed specific to
experimental needs of the times.
Over the following decades, a variety of improvements in the design and operation of gas-filled detectors
were implemented. For instance, it was learned that the proper application and selection of gas components
permitted much better operation of Geiger-Müller counters. New electrode designs permitted large detectors
to be built, some spanning over a meter in area with multiple anodes. Gas detectors have found uses as
gamma-ray spectrometers and neutron detectors and, today, gas-filled detectors continue to be used routinely
for radiation detection applications.
Better detectors were also sought that might be more efficient, less cumbersome and easier to use. It was
understood that solids absorbed radiation more effectively than gases, and so there was effort to develop a
solid-state conducting detector. Röntgen and Joffé [1913] published the first (known) observations of induced
currents in certain solids. Röntgen [1921] continued the efforts, as did many other enthusiasts such as Schiller
[1926] and Jaffé [1932]. Yet, their choices of materials were unfortunate, being mainly quartz, mica, rocksalt,
glass, and other electrically insulating materials. Hence, the results were poor mainly caused by the very
small induced currents, inadequate amplification electronics, crude counting methods, and time-dependent
material polarization.
Scintillators, materials that emit visible light when irradiated with energetic particles or photons, offered
another method to produce solid-state detectors. Scintillation materials were known since Röntgen’s initial
discovery of x rays with the BaPt(CN)4 -coated plate, yet a number of problems prevented the realization of a
practical device for decades, mainly (1) that the scintillators used had poor light yield efficiency and (2) that
there were then no practical devices available to measure or amplify the scintillation light output. Two major
developments allowed scintillators to become practical and useful radiation detectors and spectrometers,
namely the development of the photomultiplier tube (PMT) and the discovery of scintillating thallium-
doped sodium iodide (NaI:Tl). There is evidence that Leonid A. Kubetsky [Lubsandorzhiev 2006] developed
an electron amplifier that utilized secondary emission. Known as “Kubetsky tubes,” the devices constitute
an early version of the modern PMT. Independently, in 1935, a single-stage PMT was developed by RCA
that had a gain of 8 [Burle 1980]. A multistage PMT was reported by Zworykin in 1936 that was operated
by adjusting electric and magnetic fields but which proved to be impractical. Meanwhile, in 1937 Kubetsky
published the descriptions of numerous photomultiplier designs with gains as high as 106 . Within a few years,
in 1941, RCA developed and commercialized the 931A PMT that had high electron signal gains, thereby
providing a light amplification device that could be used with scintillators.
Various known organic scintillators were used in conjunction with the newly developed RCA 931A PMT
with encouraging results. However, it is Hofstadter’s discovery of NaI:Tl in 1947 that marks the beginning of
a truly practical portable gamma-ray scintillation spectrometer [Hofstadter 1948; Hofstadter and McIntyre
1950]. NaI:Tl is a bright scintillator that emits approximately 43,000 visible light photons per MeV of energy
absorbed, and the light yield as a function of energy is acceptably linear. Within a few years, commercial
NaI:Tl gamma-ray spectrometer units were available.
Despite the success of NaI:Tl as a solid-state gamma-ray spectrometer, effort still continued to develop a
solid-state version of an electron conduction device. Van Heerden [1945] demonstrated what is often referred
Sec. 1.2. A Brief History of Radiation Detectors 13

to as the first “practical” semiconductor radiation detector. In his Ph.D. dissertation, “The Crystal Counter,”
he decries the use of AgCl crystals cooled to low temperatures to detect alpha particles from a 210 Po source
[see also Van Heerden and Milatz 1950]. Shortly thereafter, CdS crystals were used to observe pulses from
gamma rays and beta particles (as reported by Frerichs and Warminsky [1946] and later by Goldsmith and
Lark-Horovitz [1949]). In 1947, Wooldringe et al., followed by Jentschke 1948, reported induced electrical
pulses from diamond samples.10
Although semiconductor detectors remained of interest, the development of NaI:Tl devices kept the status
of semiconductor detectors, then referred to as “crystal counters,” to little more than interesting gadgets.
The main problem with semiconductor devices was the unfortunate high concentrations of defects in the
crystals. The defects, which included impurities, dislocations, and intrinsic defects, caused severe problems
with charge carrier collection from the devices. With the success of NaI:Tl, it appeared that crystal counters
offered little hope for improvement, if any, to radiation spectroscopy.
Nevertheless, a variety of advances in semiconductor detectors began to occur after 1948 [see reviews by
Hofstadter 1949a, 1949b; Chynoweth 1952; McGregor and Hermon 1997]. McKay [1949, 1951] developed a
radiation detector using a point contact on a Ge semiconductor substrate. The rectifying point contact was
irradiated with alpha particles from a Po source, and this detector yielded sizeable electronic pulses on the
order of 8-12 millivolts at reverse biases between 2-10 volts. Soon after, various forms of diffused junction and
“surface barrier” detectors were developed based on Ge and Si [Dearnaley and Northrop 1966]. However, the
development that finally allowed semiconductor detectors to become serious devices for radiation detection
and radiation spectroscopy was the introduction of Li ion drifting by Pell [1960]. Li ions were electrically
drifted into Si and Ge crystals to nullify, or “compensate for,” the effects of residual impurity dopants.
Originally, university and government researchers found it necessary to construct their own custom semi-
conductor detectors, and many techniques were developed and published to build surface barrier, pn junction,
and Li-drifted detectors. However, with the success of Li drifting, a variety of semiconductor detectors be-
came commercially available by 1964. Also by this time the traditional name of “crystal counter” was
dropped and replaced with the more descriptive name “semiconductor detector.” The semiconductor de-
tectors enabled gamma-ray and particle energy identification with outstanding resolution, far better than
that achieved with scintillation detectors [Bertolini and Coche 1968; Poenaru and Vilcov 1969; Deme 1971].
Lithium drifted Ge detectors, or Ge(Li) detectors, were of more use for gamma-ray spectroscopy than the
Si(Li) detectors due to the greater atomic number of Ge (32) over Si (14), which gives Ge a higher absorption
efficiency. Both Ge(Li) and Si(Li) detectors11 needed to be operated at cryogenic temperatures near 77K to
reduce thermal noise and leakage currents. This operating criterion was especially true for Ge(Li) devices
for an added reason; if the detector warmed up, the Li would diffuse and redistribute in the crystal and the
detector would be ruined [Dearnaley and Northrop 1966; Bertolini and Coche 1968]. Hence, Ge(Li) detectors
had to be kept at cryogenic temperatures at all times, which is an obvious disadvantage.
Another method of dealing with the contaminant impurities is to remove them by various methods. Zone
refinement, one such method, had already been used to purify and remove background impurity contaminants
from a number of substances. Robert Hall at General Electric Co. (GE) suggested in 1968 that this method
might be used to purify Ge to such levels that Li drifting would no longer be necessary. Two research groups,
one at GE led by Robert Hall and another at Lawrence Berkeley Laboratory led by W.L. Hansen, developed
a method of zone refinement for Ge [Yu and Cardona 1996]. Soon high-purity Ge (HPGe) detectors became
commercially available, and over the years Ge(Li) detectors have been largely phased out for the preferable

10 Jentschke references a diamond device that was reported by Stetter [1941], thereby predating Van Heerden’s work. The device
was used to observe pulses from an alpha particle source, yet the article is unclear on many aspects of the experiment, and
the work was largely overlooked for many years.
11 The traditional pronunciation is “jelly detector” for the Ge(Li) detector and “silly detector” for the Si(Li) detector.
14 Origins Chap. 1

HPGe detectors. HPGe detectors must still be cooled to cryogenic temperatures to prevent damage from
excessive leakage currents; however, when not operating these detectors are no longer ruined if they are
allowed to warm up. As explained in a later chapter, Si(Li) detectors currently remain important as x-ray
spectrometers and are still commercially available.
Although Ge and Si have been established as important radiation detectors, the need for cryogenic
cooling is inconvenient, especially in situations where a portable device is required. Hence, the search for
semiconductor devices that can operate at room temperature remains a priority. Detectors made from
gallium arsenide (GaAs), a wide band-gap semiconductor that can be operated at room temperature, were
studied and reported as radiation counters in 1960. In 1970, Eberhardt, Ryan, and Tavendale demonstrated
the first high energy resolution semiconductor room-temperature-operated gamma-ray spectrometer. The
detector was fabricated from a high-purity, epitaxially grown GaAs crystal, and the active region of the
device was only 80 microns thick. Since then, many other, and perhaps more promising, semiconductors
have been studied. These include mercuric iodide, cadmium telluride, and cadmium zinc telluride. The main
impediment to widespread use of compound semiconductors is the difficulty of producing quality detector
crystals. It is much harder to produce defect-free compound semiconductors than it is to produce defect-free
single-element semiconductors, of which only Si and Ge are practical materials.12
A timeline of the major developments in radiation detector inventions is shown in Figs. 1.16 and 1.17.
This chart provides a snapshot up through 2010. However, this is not the end of detector history. Detector
development actively continues today and the discipline is far from being exhausted, as evidenced by many
new devices and designs produced in the past two decades. Novel approaches and designs, such as the gas
electron multiplier (GEM), have expanded the use of gas-filled detectors. New scintillation materials, such
as various lanthanide halides and elpasolites, have been developed that offer gamma-ray energy resolution
that is much better than NaI:Tl. Also, new compact photomultiplier devices based on semiconductors have
become available. Clever semiconductor detector designs have significantly reduced the effects of defects
previously impeding progress with compound semiconductor detectors. Novel detector approaches using
cryogenics have yielded devices with unprecedented energy resolution. Micro-machined semiconductors have
produced the first high-efficiency semiconductor neutron detectors. All of these devices, amongst a myriad
of other designs and technologies, some still in development, are described in chapters throughout this text.

12 There are other single element semiconductors, such as C (diamond) and Te, but these materials have intrinsic properties
that generally disqualify them. Because of its high melting point, diamond cannot be produced through traditional bulk
crystal growth processes and is generally grown as thin chemical vapor deposition (CVD) films. Unfortunately, these diamond
materials continue to have issues with defects. Further, with C having such a low Z number (6), they are simply not useful as
gamma-ray spectrometers. However, there has been some effort investigating diamond as radiation-hard particle detectors. Te
is a semiconductor, but its band gap (0.33 eV) is smaller than Ge (0.72 eV), hence such detectors would need to be operated
at cryogenic temperatures, thereby offering no significant advantage over Ge detectors.
Gas Scintillator Semiconductor

Roentgen discovers X-rays barium-platinocyanide plate


Becquerel discovers natural radiation
Thompson discovers the electron
Curies discover Po and Ra Austin, Stark report
Rutherford discovers alpha and beta rays secondary electron emissions
Villard discovers gamma rays Crookes ZnS spinthariscope
Geiger-Rutherford counter
Rutherford discovers the proton
Sec. 1.2. A Brief History of Radiation Detectors

Wilson cloud chamber


Millikan measures the charge of the electron
R
oe
nt
ge
Slepian proposes secondary n,
electron emission as amplifier Jo
ff First studies on
Roentgen e crystal counters
Sc
Bolthe invents coincidence counting lle
hi
r
Ja
Geiger-Mueller counter ffe
Kubetsky amplifier tube
Chadwick discovers the neutron
Iams, Salzburg PMT
Dunning et al. Li/B coated neutron detector
Zworykin, Morton, Malter
multistage PMT
Korff and Danforth BF3 neutron detector
first commercial PMT RCA 931A Stetter’s diamond measurements
Simpson gas-flow proportional counter

Figure 1.16. Important events in the development of radiation detectors.


Van Heerden’s AgCl device
PMT used to measure scintillator light
Frisch grid ion chamber Frerichs, Warminsky CdS device
PMT coupled to scintillator
Liebson halogen counter

1890’s 1900 1910 1920 1930 1940


1890’s 1900 1910 1920 1930 1940

Hofstadter discovers NaI(Tl) Woodridge, Ahearn, Burton diamond device


McKay Ge point contact device
flat face blue sensitive PMT
RCA 5819 Lark, Horowitz Ge np junction device
15
Gas Scintillator Semiconductor 16

3 Lark, Horowitz Ge np junction device


Batchelor - He proportional counter
Simon Ge surface barrier device
Davis Si surface barrier device
Pell introduces Li drifting in Si and Ge;
commerical Si detectors available;
negative electron affinity PMT Hilsum GaAs device
commercial Ge(Li) detectors available
phoswich detectors introduced Zanio, Autagawa, Mayer CdTe device
Charpak - multi-wire proportional counter
Hall (GE), Hansen (LBL) introduce
high purity Ge process
Eberhardt, Ryan, Tavendale - first room
temperature gamma ray spectrometers (GaAs)
Willig, Roth HgI2 and PbI2 devices

Cusano - ceramic scintillators

Melcher - discovery of LSO


Doty et al. - first CZT gamma-ray detector

Barret, Eskin, Barber - small pixel effect;


Sauli - gas electron multiplier (GEM) Luke - coplanar grid device
McGregor, Rojeski - virtual Frisch grid detectors
van Eick - discovery of LaBr3(Ce)

McGregor, Ohmes - micro pocket fission Bondarenko, Saveliev - the SiPM McGregor - microstructured neutron detectors
detectors
Bessiere, et al., elpasolite scintillators He - three dimensional gamma ray imaging

Figure 1.17. Important events in the development of radiation detectors.


Yakunin et al. perovskite x-ray detectors
Origins

1950 1960 1970 1980 1990 2000 2010


1950 1960 1970 1980 1990 2000 2010
Chap. 1
References 17

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FLAKUS, F.N., “Detecting and Measuring Radiation—A Short His-
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as a Crystal Counter.” Phys. Rev., 75, 526–527, (1949).
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HOFSTADTER, R., “Alkali Halide Scintillation Counters.” Phys. Dissertation, 1945.
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(1949a). and γ−Rays,” Physica, 16, 505–527, (1950).
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Chapter 2

Introduction to Nuclear
Instrumentation

“...that a module be developed by the National Laboratories with the intent that
the module will become standard in all of the National Laboratories and will be
duplicated by many manufacturers.”
U.S. National Bureau of Standards, 1963

Why is This Chapter Here?


In many ways this is an “orphan chapter” in that it does not discuss directly the theoretical principles or
design of radiation detectors. Consequently, it could appear at the end of the book or even as an appendix.
However, traditionally, courses designed to teach the principles of radiation detection and measurement usu-
ally have an associated laboratory component in which the actual detectors of various types are used to
demonstrate radiation detection principles. The authors have learned that for such courses students must be
introduced early to the various electronic devices they are going to use to make different radiation measure-
ments. This early introduction is essential to minimize the many (often quite creative and destructive) ways
students try to misuse the electronics to produce observable signals and measurements in the laboratory.
This chapter also serves as a historical view of how the electronics for various radiation detectors has
evolved and become standardized over the past many decades. However, the reader may safely skip this
chapter in the initial reading because little that follows critically depends on the information in this chapter.

2.1 Introduction
Nuclear instruments are designed to acquire and produce meaningful signals from radiation detectors. Almost
all radiation detectors must have electrical power applied to them in some form or fashion and, hence, it is
important to have a stable power supply.1 Detectors that operate by producing electronic signals must have
accompanying electronics that can accurately measure the magnitude of induced current or induced charge.

1 Exceptions are detectors that use radiation to produce measurable chemical changes, e.g., photographic films, or changes in
crystalline and chemical structures, e.g., color changes in crystals or material embrittlement.

19
20 Introduction to Nuclear Instrumentation Chap. 2

Often the signal from the detector must be shaped and/or amplified so that it can be manipulated by other
nuclear electronic instruments. Typically, there is also a user interface that allows one to easily interpret
the data that is being accumulated or recorded. Such an interface can assume several forms, ranging from
a simple analog meter up to a complex computer interface. The basic components for a radiation detection
system are found in all such systems ranging from small portable hand-held devices to systems with sizes of
hundreds of meters or kilometers that are used in high-energy physics experiments.

2.2 The Detector


The detector is the active element used to absorb radiation particles and subsequently produce a recognizable
signal associated with each event. Detectors may rely upon measurable phenomena, such as electronic,
thermal, or visual changes. Detector types are commonly categorized as gas-filled detectors, scintillation
detectors, semiconductor detectors, and alternate detectors. Gas-filled detectors, as the name implies, are
vessels filled with a gas, which may be under pressure or under a slight vacuum (and are covered in Chapters
9–11). Ionizing radiation interactions produce mobile charges in the gas, which, in turn, are usually identified
as an induced current or voltage caused by the motion of these mobile charges. Scintillation detectors fluoresce
when ionizing radiation interacts in the absorbing medium (see Chapters 13 and 14). These scintillation
detectors are fashioned from solid, liquid, or gaseous materials that produce measurable light when stimulated
by ionizing radiation particles. Semiconductor detectors are solid-state devices that change conductivity
when radiation particles interact in the material, mainly due to the excitation of mobile charges to higher
energy levels (see Chapters 15–16). Alternate detectors include devices that indicate the presence of radiation
by acoustical changes, color changes, temperature changes, and variety of other phenomena (see Chapter
19).
Electronic detectors in a low-level radiation environment are usually operated in pulse mode, whereas
detectors in a high radiation environment are usually operated in current mode. To understand the differ-
ence, shown in Fig. 2.1 is a common electronics arrangement for pulse mode counting. Radiation particles
interacting in the detector produce an electronic signal which can be sensed and amplified by the preamplifier
circuit. The signal from the preamplifier is then shaped and amplified further, where it either is rejected
or accepted by discriminating electronics. Afterwards, the count rate or energy spectrum is recorded and
displayed. The advantage of this method is that small currents can be converted into large voltage pulses
through the pulse shaping and amplification stages. However, the entire process involves some finite amount
of time, especially in the pulse processing stage, which defines the resolving (dead) time of the system.
Radiation particles entering the detector at a higher rate than can be processed result in dead time losses;
hence an alternate measurement method must be used when particles interact in the detector at a rate faster
than the pulses can be processed.
In current mode, the current produced in a detector is directly measured with a current meter, usually
by measuring the voltage across a load resistor through which the induced current flows. Unfortunately,
these currents for a single ionizing event can range from tens of picoamperes to a few nanoamperes. Hence,
current mode measurements are usually reserved for high radiation environments in which the signal is a
result of many, nearly simultaneous, ionizing events.
Some radiation detectors must be used in pulse mode rather than current mode. For instance, the gas-
filled ion chamber can be operated in either pulse mode or current mode, but other gas-filled detectors, such
as Geiger-Müller counters can only be operated in pulse mode. There are many other examples that are
covered in later chapters.
The detector for any single radiation measurement must be carefully chosen for the specific application.
No single device can provide all of the desired aspects of a radiation detector. When selecting a detector,
the operator must consider the radiation being measured (gamma-rays, neutrons, charged-particles, etc.),
Sec. 2.3. Nuclear Instrumentation 21

the radiation exposure rate, and the information sought (energy, count rate, etc.). Some detectors are best
suited for energy identification, others are best suited for high interaction efficiency, while still others may
provide a more economical but satisfying result. Hence, the operator must choose a detector that provides
the required information for a measurement, often from many possible sensors.

2.3 Nuclear Instrumentation


Instrumentation for the nuclear industry was specified in a 1964 report TID-20893 to the U.S. Atomic Energy
Commission (now, after many reincarnations, the Department of Energy) to what are referred to as Nuclear
Instrument Modules (NIM). Several revisions to the standard were submitted over the following years,
eventually established in the 4th revision of 1974 (TID-20893-REV-4), with an updated version described
in the 1990 report DOE/ER-0457T. The standard defines the dimensions, standard connections, and power
requirements for modular nuclear electronic components, as well as the cabinet or bin into which these
components are inserted. The NIM standard is a flexible and simple system that can incorporate many useful
detection tools, such as amplifiers, analog-to-digital converters (ADCs), counting and timing electronics,
discriminators, and power supplies. The NIM standard provides a common footprint for electronic modules
(amplifiers, ADCs, discriminators, etc.), all of which plug into a larger chassis (NIM bin). This bin must
supply ±12 and ±24 volts DC power to the modules via a backplane; the standard also specifies ±6 V DC
and 220 V or 110 V AC pins; however, not all NIM bins provide these other voltages. Shown in Fig. 2.1 is
a block diagram of components commonly used in a pulse-mode counting system, and shown in Fig. 2.2 is
a NIM bin with common components described in Section 2.5.

2.4 History of NIM Development


Early nuclear instruments were composed of vacuum tube circuits within a standardized 19-inch wide chassis.
The components each had their own DC power supply and each connected directly to AC power. These
components easily installed in standard 19-inch wide instrument racks. Hence, there was no issue with
interchangeability between components, mainly because each unit operated independently.
The invention of the transistor in 1948 later allowed the electronics to be built much more compactly. Fur-
ther, the overall efficiency and heat load was significantly less for transistorized components. Yet, these early
transistorized nuclear instruments were built in a similar fashion as were their vacuum-tube counterparts,
designed for large 19-inch wide containers. It was eventually realized, however, that these transistorized
electronic components could be built as smaller and more efficient modular units, thereby eliminating the
need for a single 19-inch wide chassis. Many independent laboratories and commercial companies began
designing and constructing various different modular electronic component systems.
Two such systems, advanced at the time, were the systems developed by the European Organization for
Nuclear Research (CERN) and the United Kingdom Atomic Energy Research Establishment. The European
Standards community on Nuclear Electronics (ESONE), founded in 1961, also began working on a new
standardized modular system. Along with these systems, numerous commercial companies began working
on various modular nuclear electronics systems. Further, the independent U.S. national laboratories began
developing modular nuclear electronics systems for their own purposes. As a result, numerous different
nuclear electronics systems were under development, none of which was compatible with any of the other
systems. Overall, research at nuclear laboratories was seriously limited by the compatibility of instruments,
and researchers were forced to invest in numerous different modular nuclear components.
To remedy this divergent development of nuclear modules, the U.S. National Bureau of Standards (NBS),2
in a 1963 report to the U.S. Atomic Energy Commission (AEC), recommended that the U.S. national

2 The National Bureau of Standards is now the National Institute of Standards and Technology (NIST).
22 Introduction to Nuclear Instrumentation Chap. 2

oscilloscope

discriminator
detector preamplifier amplifier or SCA counter/timer

040657
g-ray
1

+ - 2
power supply MCA

Figure 2.1. The basic components of a pulse-mode electronic detection system. A detector is powered
by a bias supply or power supply usually through the preamplifier. The induced electronic signal from the
detector is shaped and amplified through the preamplifier and amplifier circuits. The signal can be observed
and monitored with an oscilloscope. When used as a basic counter, the shaped signal pulse is routed through
a discriminator or single channel analyzer (SCA) and then into a counter/timer (route 1). When used as
a spectrometer, the shaped signal pulse is routed into a multichannel analyzer (MCA) in which the pulse
amplitudes are sorted and categorized according to the pulse heights (route 2).

laboratories develop a modular system to be duplicated by commercial manufacturers. The U.S. AEC
convened a meeting of representatives from several national laboratories on Feb. 26, 1964 to determine if
such a task was of interest to the laboratories. In agreement, the AEC Committee on Nuclear Instrument
Modules was established, composed of members from all AEC national laboratories and a few other prominent
nuclear laboratories.
The first NIM Committee meeting was held on March 17, 1964, with follow-up meetings over several
ensuing months. The committee studied the advantages and shortcomings of the existing modular systems,
and a system similar to the CERN design was eventually developed. The prototype bins were manufactured
by Oak Ridge National Laboratory (ORNL), Lawrence Radiation Laboratory in Berkeley and Lawrence
Radiation Laboratory in Livermore.3 These early prototypes were studied at later meetings of the NIM
Committee, eventually leading to a recommended design. Final details were resolved by the NIM Executive
Committee with representatives from the U.S. NBS, ORNL, Lawrence Radiation Laboratory in Berkeley, and
with later added members from Princeton-Pennsylvania Accelerator and Brookhaven National Laboratory
(BNL). The final specifications were published in July 1964, and later updated versions of the specifications
were published in 1966, 1968, 1969, and 1974. The standard was well received, with the first commercial
NIM components being available by November 1964. During 1965, numerous more NIM instruments became

3 The Lawrence Radiation Laboratory in Berkeley is now the Lawrence-Berkeley National Laboratory and the Lawrence Radi-
ation Laboratory in Livermore is now the Lawrence-Livermore National Laboratory.
Sec. 2.5. NIM Components 23

Figure 2.2. A typical measurement system in which various NIM components are installed into a
NIM bin shown to the right. This NIM bin contains several nuclear instrument modules, including
a power supply, a pulser, an amplifier, an SCA, and a counter/timer. The detector, to the left of
the NIM bin, is a NaI:Tl device with the preamplifier attached to the detector back. The system
is also attached to an oscilloscope, shown on top of the NIM bin. The detector is also connected
to a computer-based MCA, which shows a spectrum of 137 Cs gamma rays on the monitor, behind
the keyboard. The 137 Cs gamma ray check source is located directly beneath the NaI:Tl detector.

available, and NIM components accounted for over 95% of all modular nuclear instruments produced in the
U.S. in the immediate years following 1967. The NIM standard was again revised in 1990, to make the
standard compatible with existent technology and manufacturing processes, as described in Department of
Energy (DOE) document DOE/ER-0457T.

2.5 NIM Components


Commercial manufacturers offer a variety of NIM components for radiation detection applications. Many
of these modules are versatile and can be used for general radiation counting applications. There are also
special NIM modules optimized for narrowly applied or special applications. Overall, the list of common
NIM components include a NIM bin and power supply, a detector voltage supply, preamplifier, amplifier,
discriminator, counter, timer, and often a data analyzer. Described in the following sections are the basic
properties of these components. Further details on the design and operation of NIM components and other
nuclear electronics can be found in Chapter 22.

2.5.1 The NIM Bin


The container for NIM components is traditionally referred to as a NIM bin. The NIM bin is used as the
power supply docking port for most NIM components, except for a few high voltage power supplies that
24 Introduction to Nuclear Instrumentation Chap. 2

plug directly into a 120 VAC wall socket.


NIM sockets The most common NIM bin size, shown in
Fig. 2.3, has space for 12 single-width NIM
components, as specified by DOE/ER-
0457T. There are also more compact NIM
bins with only 4 single width slots. These
smaller NIM bins are typically used for
portable measurement situations that re-
quire only a few NIM instruments. A
power supply is placed behind the instru-
ment slots in a NIM bin. This unit pro-
DC voltage
NIM slots vides ±6 volts DC, ±12 volts DC, and ±24
test jacks
volts DC to the NIM sockets and voltage
jacks,4 as well as 117 volts AC. Power is
commonly rated between 150–160 W for
the larger power supplies, although lower
power models rated at ∼95 W are avail-
able (usually for models that do not of-
NIM bin
fer the ±6 volt DC option). The NIM
power supply
bin sockets and pin assignments conform
to the specifications outlined in DOE/ER-
0457T. Test jacks in the front of the NIM
bin provide convenient access to monitor
the DC voltage, and can also be used to
conveniently supply power to custom elec-
tronics. Modern power supplies are filtered
from electromagnetic interference (EMI),
Figure 2.3. (top) Front view of a NIM bin, showing the NIM slots
and power sockets. (bottom) Back view of a NIM bin, showing the
are short-circuit proofed, thermally pro-
power supply. tected, and provide stable power required
for NIM components. Usually NIM bins
have warning indicators that inform the operator if the power supply is approaching the temperature limit.

2.5.2 Detector Power Supplies


Detectors that operate with the NIM system typically produce an electronic output and, therefore, require
a power supply of their own. Traditionally, the majority of such NIM power supplies for detectors apply a
high voltage to the detectors.5 Stability of the supply voltage is of particular importance in high-resolution
measurements systems. High-voltage power supplies are used to operate detectors that do not suffer changes
in capacitance as a function of voltage, such as gas-filled and scintillation detectors. High-voltage bias
supplies are usually used for semiconductor detectors, in which the operating voltage can affect the detector
capacitance.
High Voltage Power Supply
The high voltage power supply, as the name implies, supplies high voltage to the detection device, and
can supply it with either positive or negative polarity. Typically, the voltage is applied to the detector

4 Some models provide only ±12 VDC and ±24 VDC.


5 Recently,there has been a move toward special detector systems based on semiconductor photon detectors that operate on
lower voltages. These detectors, such as avalanche photodiodes, are discussed in Chapter 14.
Sec. 2.5. NIM Components 25

Figure 2.4. (left) A common all-purpose HV


power supply used for gas-filled and scintillation
detectors. (right) A dual source DC bias supply
used for smaller semiconductor detectors, such as
silicon surface barrier detectors.

across a load resistor with the connection routed through the preamplifier unit. Also, a power supply often
has a meter indicating the applied voltage, which is reasonably accurate because the detector resistance
is typically much greater than the preamplifier load resistance. HV power supplies are available with the
maximum voltages exceeding 3.5 kV. Because PMTs and gas-filled devices need relatively high power, a HV
power supply is plugged directly into a wall socket, although many models have rails that allow the power
supply to slip into a NIM bin for convenience. A HV power supply is shown in the left-hand side of Fig. 2.4.
High Voltage Bias Supply
For semiconductor detectors, the power supply is generally referred to as a “bias supply.” As with a HV
power supply, the bias supply provides a choice of positive or negative high voltage to the detector. However,
this power supply does not have a meter, but rather only a dial indicator for the total applied voltage to the
system.
Because the system includes load resistances in series with the detector, there is a voltage drop across
this resistance, which reduces that applied to the detector. Thus, a meter indicating total voltage would be
misleading. Instead jacks are provided that allow determination of the bias current. Because the series load
resistance is known, the voltage applied to the detector, which is less than the total, can also be determined.
Bias supplies are available for which the maximum allowable voltages can exceed 5 kV. Because typical
26 Introduction to Nuclear Instrumentation Chap. 2

power supply
from amplifier
power supply timing signal test signal
input input input

detector voltage/
signal input

signal out
(energy)

Figure 2.5. (left) Front view of a common charge-sensitive preamplifier, showing the safe high
voltage (SHV) connector for the detector and the nine pin D-subminiature connector for the
preamplifier power. (right) Back view of a the same charge-sensitive preamplifier, showing the
connector terminals for the power supply, pulser input, timing input, and the output signal.

detectors are highly resistive and draw little current, the power requirement of the bias supply is low and,
consequently, most bias supplies are plugged directly into the NIM bus for power, unlike the HV power
supply. A HV bias NIM module is shown in the right-hand side of Fig. 2.4.

2.5.3 Preamplifier
A preamplifier unit has two basic purposes, namely (1) to provide low noise coupling of the detector to
the string of amplifier and readout electronics, and (2) to produce a first stage of signal amplification. The
preamplifier thus acts as a filter against objectionable line noise that may alter the input signal. Pream-
plifiers are designed to be either current sensitive, voltage sensitive, or charge sensitive. Optimum detector
performance is obtained when the user selects the proper preamplifier matched to the type and characteris-
tics of the detector and the analysis electronics. The general application of these preamplifiers are described
here, with details on the design and operation reserved for Chapter 22.
Voltage-Sensitive Preamplifiers
Voltage-sensitive preamplifiers are so named because they tend to respond to and linearly amplify the
voltage input from the detector into the preamplifier circuit. As discussed in Chapter 8, the voltage input
Vin into the preamplifier from the detector is generally an inverse function of the detector capacitance,
Vin ≈ Qi /Cd , where Qi is the charge induced by the motion of electrons and ions excited in the detector by
a radiation interaction event and Cd is the combined capacitance of the detector and coupling cables. The
preamplifier output is usually defined by the feedback resistors, where for a typical inverting configuration
Vout ≈ −(Rf /RL )Vin , where Rf is the feedback resistance and RL is the input load resistance.
For many detectors, the capacitance remains constant for different applied operating voltages Vo ; hence
the preamplifier output Vout is mostly linear with respect to the charge excited in the detector regardless of
the voltage applied to the detector. Examples include gas-filled detectors and scintillation detectors that are
coupled to photo-multiplier tubes.
Charge-Sensitive Preamplifiers
There are some detectors that change capacitance as voltage is applied, particularly semiconductor diode
detectors. These semiconductor detectors have active regions that increase with applied operating voltage,
which, in turn, causes the capacitance Cd to decrease with increasing voltage. As a result, the preampli-
fier output changes with a varying operating voltage for identical induced charge Qi . By redesigning the
preamplifier feedback circuit, the capacitive component of the detector Cd can be minimized compared to
Sec. 2.5. NIM Components 27

the feedback capacitance Cf of the preamplifier, thereby, effectively rendering the preamplifier output al-
most entirely dependent upon the induced charge Qi . Hence, for semiconductor diode detectors, the voltage
output Vout is largely dependent only upon the induced charge Qi and feedback capacitance Cf , where
Vout ≈ −AVin ≈ −Qi /Cf , where A is the preamplifier gain. Commercial charge sensitive preamplifiers are
designed for optimum performance when matched to specific ranges of detector capacitance. Hence, it is ad-
vised that the user consult the preamplifier specification sheets to properly match detectors to preamplifiers.
A common commercial charge sensitive preamplifier is shown in Fig. 2.5.
Current-Sensitive Preamplifiers
As the name implies, a current-sensitive preamplifier is designed to measure the instantaneous current flowing
from a detector. The configuration is seldom used for most detector applications; however, on rare occasions
a preamplifier with a fast rise time for timing applications is needed, and a current sensitive preamplifier is
required. The current sensitive configuration requires that the input impedance be low and the preamplifier
gain A be large. These conditions can be realized by using the general design of a voltage sensitive preamplifier
and reducing the load resistance at the input of the preamplifier. Note that the Johnson noise6 can be high
unless the feedback resistor in the preamplifier circuit is Rf ≥ 109 Ω. If the preamplifier input impedance is
50 Ω, the current sensitive preamplifier will convert the input current Iin to an output voltage Vout described
by Vout = Iin (50Ω) A.

2.5.4 Amplifier
The amplifier unit has two main purposes, namely, (1) pulse shaping and (2) pulse height amplification.
The pulse at the output of the preamplifier typically has a fast rise time with a slower falling tail with the
timing characteristics determined by the leading and trailing time constants. This pulse is then integrated
and shaped by the amplifier to provide a Gaussian-like pulse that is far easier to manipulate with counting
electronics that are placed further down in the pulse processing system. The amplifier, depending on its
design, may allow the user to change rise times, decay times, and pulse width. Further, the gain on an
amplifier has both course and fine adjustments, important features needed when calibrating the system.
Lastly, the NIM standard allows for a 10-volt maximum output from the amplifier, i.e., any pulses whose
amplitude is larger than 10 volts is “clipped” at 10 volts. Hence, it is wise to adjust the amplifier gain
so that the largest expected output pulses are less than 10 volts; otherwise, the clipped signal may not be
recognized or counted.

2.5.5 Oscilloscope
Although an oscilloscope is not part of the NIM system of instruments, it is a fundamental and important
piece of equipment with which all NIM users should become familiar. The oscilloscope allows the user to
determine how the system is manipulating the electronic pulses at every stage of the system by simply
hooking into that portion of the pulse processing system with a “tee” connector. It can be used to measure
pulse heights, pulse widths, repetition rates, pulse symmetry and variety of other values that allow for
trouble-shooting and system calibration.

2.5.6 Pulse Discriminators


A simple discriminator is used to reject pulses outside set pulse-amplitude boundaries, thereby passing only
pulses of certain voltages that are of interest. The electronic pulses emerging from the amplifier are indicative
of the amount of energy deposited within the detector, typically linear with energy in well-designed systems.
Hence, once calibrated, the final signal pulse height is a measure of the energy absorbed in the detector.

6 Johnson noise is the electronic noise generated by the thermal agitation of the charge carriers inside an electrical conductor.
28 Introduction to Nuclear Instrumentation Chap. 2

The discriminator allows the user to select a voltage at a lower level discriminator (LLD) threshold, below
which pulses are rejected. In older discriminators, any signal above the LLD is passed. However, some newer
systems reject pulses that exceed the 10-volt upper limit. Often a “discriminator” unit has only an LLD,
whereas the single channel analyzer (SCA) has both an LLD and an upper level discriminator (ULD). The
ULD rejects signal pulses that exceed the set threshold. Hence, the SCA allows the user to pick a voltage
region (or energy region) of interest defined by lower and upper energy thresholds, and pass only those signal
pulses that fall within those boundaries.

2.5.7 Counter/Timer
Voltage pulses that pass through the discriminator or SCA are usually routed to a counter/timer. The
function of the counter/timer is to record the number of radiation induced pulses within a predetermined
amount of time. Hence, a count rate from a radiation source can be determined. Most counter/timers can
be set to automatically count for a preset amount of time and stop so as to reveal the number of pulses or
counts obtained within that time period. Conversely, they can be set to record a certain number of counts
and stop when that limit is obtained to reveal the time required for the measurement. Counter/timers are
common instruments used for radiation measurement and dosimetry.

2.5.8 Pulse Generator


A valuable piece of equipment that assists with calibration of the radiation counting system is the pulse
generator, and is commonly referred to as a pulser. Pulsers provide accurate voltage test pulses into the
radiation detection system. The pulses can be set to have different shapes (tail pulse being the most
common), decay times, pulse frequencies, and amplitudes in order to calibrate the amplifier, MCA, SCA, or
counter/timers. The test pulses can also be used to help determine system dead times and system electronic
noise. Although not necessary to operate a radiation counting system, they are quite valuable when first
configuring the system and calibrating it for radiation measurements. Further, it is typical that a pulser
be operating during spectroscopic radiation measurements in order to have a comparison peak for system
noise determination. Typically the pulser peak is set to an MCA channel that does not interfere with the
accumulated radiation spectrum.

2.5.9 Coincidence Modules


There are many applications that require the measurement of events that occur in two separate detectors
within a given time interval Δt. Examples include identifying the simultaneous arrival of photon-photon or
photon-particle events, positron lifetime studies, decay scheme studies. Such measurements are commonly
referred to as coincidence measurements. By contrast there are some measurements that require the opposite
condition, i.e., when two radiation events are recorded within Δt are rejected. Such measurements are referred
to as anti-coincidence measurements. Regardless, the main function of a coincidence module is to discern
the arrival of two or more radiation particles in separate detectors within some preset time interval Δt.
In practice it is not possible to analyze coincidence events with 100% confidence due to the uncertainties
associated with the statistical nature of radiation emissions. Statistical timing errors may occur from the
detection process and uncertainties in the electronics resulting from timing jitter, amplitude walk, and noise,
all of which lead to statistically variable time delays between processed events. A simple coincidence circuit
solves this problem by essentially summing the two input pulses, passing the resultant sum pulse through a
discriminator level, and generating an output pulse when the two input pulses overlap.
The period of time in which the two input pulses can be accepted is defined as the coincidence resolving
time, and is determined by the width of the pulses, τ , such that the resolving time is equal to 2τ . A
coincidence analyzer produces a logic pulse output when the input pulses, on the active inputs, occur within
Sec. 2.5. NIM Components 29

the resolving time window selected on the front panel. Because detector events occur at random times,
accidental coincidences can occur between two pulses which produce background in the coincidence counting.
The rate of accidental or random coincidences rR is given by

rR = r1 r2 (2τ ), (2.1)

where r1 and r2 are the count rates observed by the two detectors.
The number of counts in the detectors depends upon the experiment and the detectors, so the best way to
reduce accidental coincidences is to make the resolving time as small as possible. However, the resolving time
cannot be reduced below the amount of time jitter in the detector pulses without losing true coincidences,
so the type of detector determines the minimum useful resolving time.

2.5.10 Time-to-Amplitude Converters


There are some radiation measurements in which the time interval between two separate events is sought.
A time-to-amplitude converter (TAC) measures the time delay between two events Δt and converts it into
a voltage output between 0–10 volts. The magnitude of the output voltage is linearly proportional to Δt.
These pulses can be displayed as a pulse height spectrum, thereby yielding the average delay and the timing
resolution defined as the full width at half maximum (FWHM) of the pulse height spectrum.

2.5.11 Analog-to-Digital Converters


An analog-to-digital converter (ADC) generates a digital “word” proportional to the amplitude of an input
pulse. In nuclear applications, ADCs are used to digitize the output signals from spectroscopy amplifiers.
Because these amplifiers generate output pulses whose amplitudes are directly proportional to the energies
of the incident radiation, the ADC can be used with an amplifier and a multichannel analyzer (MCA) to
generate energy distributions (spectra) of the radiation emitted by radioactive samples.

2.5.12 Photomultiplier Tube Base


The photomultiplier tube (PMT) base is a separate electronic unit and not a NIM bin module and is used to
supply voltage to a PMT. PMTs are vacuum tubes commonly coupled to a scintillating detection medium,
which might be a solid, liquid, or gas. Scintillation light excited by radiation absorbed in the scintillator
detector may strike the photosensitive cathode of the PMT and eject an electron into the tube. Beyond the
light sensitive cathode, a series of metal plates or meshes, called dynodes, are biased with voltage in order to
attract and accelerate electrons. These electrons strike the dynode and knock off more secondary electrons
than were incident on the dynode, thereby amplifying the signal that increases with the number of dynodes
in the PMT. The PMT base divides the applied voltage evenly among these dynodes, with ten stage dividers
being common amongst commercial vendors. The output of the PMT base can be coupled to a preamplifier
or, in some models, the preamplifier may be incorporated within the PMT base. Some PMT bases allow
adjustment of the gain and applied bias in order to achieve optimal detector performance.

2.5.13 Multichannel Analyzer


The multichannel analyzer (MCA) measures the pulse heights emerging from the amplifier with high precision
for many pulses, one after the other, and creates a histogram of small voltage intervals or bins along the
abscissa (x-axis) and number of observed pulse heights within each interval along the ordinate (y-axis).
In the NIM standard the maximum pulse height is 10 volts so the amplifier gain must be set so that no
pulse heights of interest exceed this limit. The voltage measurement is made with a quick analog-to-digital
converter and the subsequent manipulation and storage is today done with conventional computer code
and memory. Because the underlying analog-to-digital converters and computer hardware are binary, the
30 Introduction to Nuclear Instrumentation Chap. 2

Figure 2.6. Differential pulse height spectrum of gamma rays emitted by the radioactive decay
of 152 Eu, 154 Eu, and 155 Eu as measured by a high purity germanium (HPGe) semiconductor
detector.

first MCAs divided the ten-volt span into a selectable number of bins that are increasing powers of 2 and
this approach is still used. The bins are called channels that range from as low as 128 in number to 4096
or even more. For typical scintillation or gas filled detectors 1024 or 2048 channels are sufficient, but for
higher resolution semiconductor detectors pulses are typically collected in 4096 or 8192 bins. The pulse
height spectrum that is formed from radiation induced pulses forms a histogram on the MCA output display,
usually a computer screen. The histogram represents the voltage distribution of pulse height amplitudes
provided by the detector, where the voltage pulses are linearly related to the radiation energy absorbed by
the detector for each event. Hence, the pulse height spectrum is a relative measure of the spectroscopic
energy distribution absorbed in the detector. Overall, the MCA performs the function of numerous SCAs in
series as well as a counter/timer. Modern MCAs can be set with over 16000 channels spread over 10 volts, a
requirement for radiation spectroscopy applications with ultra-high resolution. Shown in Fig. 2.6 is a MCA
differential pulse height spectrum of a mixed Eu source (152 Eu, 154 Eu,155 Eu) as taken with a high purity Ge
(HPGe) detector. Details of various types of MCAs are reserved for Chapter 22.

2.5.14 Other NIM Components


Although the main NIM (or CAMAC) components commonly used in a detecting system are listed above,
there are many other NIM components that can be used for special counting purposes. Such units include
timing modules, coincidence modules, delay lines, time-to-amplitude converters (TAC), and analog-to-digital
converters. There are also many variations of those NIM components discussed in the previous sections. The
user should consult the specifications regarding the NIM components to determine which modules are best
suited for the experiments or measurements to be made.
Sec. 2.6. CAMAC 31

2.6 CAMAC
For more complex detection systems, as may be encountered at large research facilities and high-energy
accelerator centers, there is another international standard for modularized electronics, namely, Computer
Automated Measurement And Control (CAMAC), which defines a standard bus for data acquisition and
control. The interface system, upon which this standard is based, was developed by the ESONE Committee
of European Laboratories with the collaboration of the NIM Committee of the US Department of Energy
(DOE) [ESONE, 1964; CAMAC, 1972]. This standard is based on ERDA Reports TID-25875, July 1972
(corresponding to ESONE Report EUR 4100e) and TID-25877. The standard defines the mechanical con-
struction and electrical dataway for the modules. The CAMAC also includes the IEEE standards of 583
(the basic CAMAC design), 595 (serial highway system), 596 (parallel branch highway system), 675 (auxil-
iary crate controller), 683 (block transfer specifications), 726 (real-time BASIC computer language) and 758
(FORTRAN computer language subroutines for CAMAC).
The container for instrumentation modules is referred to as a ‘crate’ or ‘CAMAC crate.’ The CAMAC
bus allows data exchange between plug-in modules (up to 24 in a single crate) and a crate controller, which
then interfaces to a PC or to a VME-CAMAC interface. The original standard was capable of one 24-bit
data transfer every μs. Later a revision to the standard was released to support shorter cycles which allow a
datum transfer every 450 ns. A follow-up on upwardly compatible standard Fast CAMAC allows the crate
cycle time to be tuned to the capabilities of the modules in each slot. Typically, CAMAC components are
significantly more costly than NIM components, and are best used when computer automation is necessary.
Regardless of the standard, both NIM and CAMAC systems use basic components to operate and manipulate
data from radiation detectors.

2.7 Nuclear Instruments other than NIM or CAMAC


Although NIM electronics are popular and still in widespread use, most of the systems that use NIM elec-
tronics are not considered portable. However, there are integrated components available as handheld or
totable instruments. Many of these instruments, or survey meters, consist of a battery-operated unit with
a detachable detector (see Fig. 2.7). The monitoring unit may have an analog or digital display that con-
veys information regarding the radiation exposure or the energy signature, and often has a dial selectable
radiation exposure range feature.
Portable instrumentation is available for gas-filled, scintillation, and semiconductor detectors, and range
in complexity from simple radiation counters to cryogenically cooled high-resolution energy spectrometers.
Some relatively new instrumentation that has become available include miniature Geiger-Müller counters
the size of key-chain holders, compact solid state VLSI7 detector packages, to sophisticated 3-dimensional
imaging devices capable of identifying radioactive sources by energy and location.
Although these devices may have special operating electronics and features, the same basic pulse pro-
cessing and signal recognition electronics described available for NIM components are usually a part of the
detector package. For instance, a handheld rate meter will typically have a power supply, amplification
and shaping, pulse discrimination, and a visual output much like a NIM system, but instead in a compact
handheld platform. Some examples of these systems are presented in many of the following chapters on
detectors.

2.8 Cables and Connectors


The proper choice of cables and connectors used with nuclear instrumentation is influenced by signal ve-
locity, instrument impedance, operation temperature, radiation environment, and mechanical environment.

7 Very large scale integration.


32 Introduction to Nuclear Instrumentation Chap. 2

Figure 2.7. Two commercial handheld portable gas-filled detectors. The


detector on the left is an ion chamber manufactured by Eberline, and the
detector on the right is a Geiger-Müller counter attached to a rate meter, both
manufactured by Ludlum.

Although numerous variations exist, there are a few standard choices for cables and connectors used in the
nuclear industry. Briefly described here are some of those choices. For a more detailed discussion on cables
and connectors for nuclear measurements, the reader is referred to Chapter 22.

2.8.1 Cables
Signal transmission of voltage pulses is most often done with coaxial cables. Such cables have a central con-
ductor, around which is an insulating dielectric material. A second conducting layer is wrapped around the
dielectric, over which a protective insulator is often applied. Common dielectric materials include polyethy-
lene and TeflonTM . For special radiation environments, cables with mineral dielectrics may be a wise choice.
The propagation speed v of a signal in a cable is dependent upon the dielectric and magnetic properties
of the internal insulating materials separating the central conductor from the outer conductor, and is given
by
1 1 c
v= √ =√ = √ , (2.2)
μ μr r 0 μ0 μr r

where r is the relative permittivity, μr is the relative permeability and, by definition, 0 μ0 = c−2 . Most
often, μr ≈ 1, hence the wave propagation speed becomes primarily dependent upon the relative permittivity.
Electric waves propagate as transverse electro-magnetic (TEM) waves, meaning that the electrical and
magnetic fields are perpendicular to the direction of wave propagation. At some “cutoff” frequency, other
modes can propagate, those being transverse magnetic (TM) and transverse electric (TE), which do not
Sec. 2.8. Cables and Connectors 33

necessarily travel at the same wave velocity, thereby potentially causing undesirable interference. Hence, it
is best to operate within the specified bandwidth of the cable.
Historically, conductor investigations indicated that wave attenuation is minimum at characteristic
impedances of 77 ohms, the breakdown voltage is greatest at 60 ohms and the power-carrying capacity
is maximized at 30 ohms. The widespread use of 75 ohm and 50 ohm cables comes from a compromise
of these properties. “Radio Guide” (RG) cable is named from the defunct military specification for cable
identification, but is commercially still in common use. RG cables have typical characteristic impedances
between 50 and 93 ohms. A table of values for various cables can be found in Chapter 22.
Finally, the perils of mixing connectors that are mechanically different is fairly obvious while mixing
cables of components of different impedances is more subtle, but can be equally problematic.

2.8.2 Delay Lines


Under some circumstances it is necessary to delay the signal from a detector before it enters the analyzing
electronics. For instance, a coincidence measurement may be desired for two different types of detectors,
but the signal processing times are different for the two devices. A delay line can be used to retard the
progression of the faster signal, thereby allowing coincident events to arrive at the same time. A simple
delay line consists of a long coaxial cable where the propagation time per unit length of cable is
√ 
1 μr r LC
td = = = , (2.3)
v c d2
where d is the cable length, L is the cable inductance, and C cable capacitance. For typical coaxial cables
that have polyethylene as the insulating filling (r  2.25), the delay time is approximately 5 nanoseconds
per meter. There are special cables designed as delay lines that have spiral conductors to increase the time
delay per unit length, thereby shortening the required cable.
Delay lines not only cause a delay in the arrival time of a signal, but also can attenuate the signal as it
travels down the cable. If the delay line is purposely shorted at the output terminal, then the signal can
be reflected back, inverted in form, towards the input terminal. As a result, the combined attenuation and
reflection of the original signal can be used to alter the final output electronic signal to a desirable outcome,
referred to as single delay line pulse shaping. The method is discussed in more detail in Chapter 22.

2.8.3 Connectors
Bayonet Neill-Concelman connectors, most often referred to as BNC connectors, are quick disconnect RF
connectors designed for use with coaxial cables (see Fig. 2.8). Cables commonly used with BNC connectors
for nuclear measurements are RG-58 and RG-59. BNC connectors can be acquired with a characteristic
impedance of 50 ohms or 75 ohms, where it is important to match the impedance of the connector to that of
cable impedance to minimize signal reflection. Although typically rated for voltage applications below 500
V, some BNC connectors can be acquired with ratings up to 900 V.
Miniature High Voltage (MHV) connectors are RF connectors for coaxial cable (see Fig. 2.9). They have
a similar appearance to BNC connectors, except that the insulation around the male pin protrudes slightly
out of the MHV connector, whereas the insulation around the male pin of a BNC connector does not. BNC
and MHV connectors do not match. MHV and BNC connectors are not interchangeable, and damage could
occur if a BNC connector is mated to a MHV connector.8
MHV connectors have potential ratings up to 5000 V DC at 3 A. MHV connectors were at one time
popular for detectors requiring applied voltages exceeding that of BNC specifications. Although still in

8 Oneauthor discovered the aftermath of a student’s amazing feat of forcing a male MHV connector onto a female BNC
connector, a result that rivals spot welding as a process to permanently fuse electrical connectors together.
34 Introduction to Nuclear Instrumentation Chap. 2

Figure 2.8. Male and Female BNC con- Figure 2.9. Male MHV connectors. No-
nectors. tice the slight insulator protrusion.

use, a MHV connector has design issues, namely, a user can be exposed to ungrounded high voltage during
disconnection; hence, SHV connectors (discussed below) have largely displaced the once popular MHV
connectors.
Safe High Voltage (SHV) connectors are RF connectors designed for use with coaxial cables. Similar
in design to a BNC and/or an MHV connector, the male SHV connector has the distinctive feature of a
shielded insulator protruding significantly from the connector body (see Fig. 2.10). The protruding insulator
on a male SHV connector remedies the safety issues of an MHV connector by preventing contact with the
high voltage conductor. Further, the design eliminates the chance of mismatching a high voltage line to a
low voltage connector, as can happen by misidentifying an MHV as a BNC. Most SHV connectors are rated
for 5000 V and 5 A.

Figure 2.11. Female (left) and male


Figure 2.10. Male (left) and female (right) N-type connectors, showing (top) 75
(right) SHV connectors. Ω and (bottom) 50 Ω variants.
Problems 35

The “N” connector, named after Paul Neill of Bell Laboratories, is a weatherproof RF connector for use
with coaxial cables (see Fig. 2.11). The connector is somewhat rugged with a threaded system rather than
a bayonet connection system. N connectors can be used with RG-8, RG-58, RG-141, and RG-225 cables. N
connectors come in 50 ohm and 75 ohm variants, and are typically rated for 1000–1500 V. In general, 50
ohm and 75 ohm variants are not interchangeable, and damage can occur if a 50 ohm N connector is mated
to a 75 ohm N connector.
The “C” connector, presumably named after inventor Carl Concelman of Amphenol Corp., is a bayonet
style RF connector that resembles that of a BNC connector, but is considerably larger in size (see Figs.
2.12 and 2.13). C connectors are relatively weatherproof and are often employed with portable survey
instrumentation. C connectors have either 50 ohm or 75 ohm impedance, and are typically rated up to 1500
V and 2 A. The actual insulator resistance is greater than 5 GΩ. C-type 50 ohm connectors can be used
with 75 ohm cable with little loss at frequencies below 300 MHz. The recommended operating temperature
range is between −65◦ C and 165◦ C.
The High-Voltage N-Type (HN) connectors are threaded weatherproof coaxial connectors designed to
withstand temperature and mechanical stresses. The connectors typically are designed with a characteristic
impedance of 50 ohms with a voltage rating of 1500 V. Operational temperature range is −65◦ C to +165◦C.
HN connectors are often employed with detector instrumentation used for nuclear reactor power monitoring.

male BNC

male C-type

Figure 2.12. Comparison of a C-type connec- Figure 2.13. Female and male C-type con-
tor with a BNC connector. nectors, showing (top) 75 Ω and (bottom) 50 Ω
variants.

LEMO connectors, named after company founder Léon Mouttet, are push-pull miniature coaxial con-
nectors with significantly smaller diameters than BNC or other common coaxial connectors. These compact
connectors can be employed for instrumentation where little space is available for multiple connectors. The
50 ohm LEMO 00 series connectors are rated at voltages above 2000 V with limit of 4 A, and they are often
used in conjunction with NIM and CAMAC instrumentation.

PROBLEMS

1. Explain the purpose behind implementing the NIM system.

2. Common RG-58/U cable has a characteristic impedance of 50 ohms per meter and characteristic capaci-
tance of 93.5 pF per meter. Calculate the length of cable required to delay a signal by 0.5 microseconds.
36 Introduction to Nuclear Instrumentation Chap. 2

3. What is the upper limit for signal voltage in a NIM system? What happens if a signal greater than the
limit passes into a NIM component such as a SCA?

4. If the standard for the upper limit for signal voltage were 10 mV, rather than the 10 V of the NIM
standard, then only a preamplifier would be necessary to provided any needed signal amplification and,
thus, would eliminate the need for an additional amplifier. Why is this low voltage limit not a good
idea?

5. What is the voltage width of each bin in a MCA with (a) 128 channels and with (b) 4096 channels?

6. Although Oliver Heaviside invented and patented the coaxial cable in 1880, almost all early work on
the development of radiation detectors and the important atomic-level discoveries in the first half of the
twentieth century, simply used wires (often bare!) for making electrical connections. So why are coaxial
cables so important in today’s detector techology?

7. Today with ultra-large-scale integrated circuits, tens of billions of electronic components can be placed
on a small chip of silicon. Indeed a complete PC, no larger than the tip of a finger, has been fabricated.
Why have electronics for radiation detectors not experienced a similar revolutionary reduction in size?

REFERENCES
American National Standard for Signal Connectors for Nuclear IEEE STANDARD, 596-1982 IEEE Standard Parallel Highway In-
Instruments, ANSI N3.3-1968, New York: American National terface System (CAMAC), IEEE, 1982.
Standards Institute, 1968.
IEEE STANDARD, 675-1976 IEEE Standard Multiple Controllers
American National Standard Nomenclature and Dimensions for in a CAMAC Crate, IEEE, 1982.
Panel Mounting Racks, Panels, and Associated Equipment,
IEEE STANDARD, 683-1976 IEEE Recommended Practice for
ANSI N83.9-1968, New York: American National Standards In-
Block Transfers in CAMAC Systems, IEEE, 1976.
stitute, 1968.
IEEE STANDARD, 726-1982 IEEE Standard Real-Time BASIC
CAMAC, A Modular Instrumentation System for Data Han-
for CAMAC, IEEE, 1982.
dling - Description and Specification, European Atomic En-
ergy Community, EURATOM Report EUR 4100e, Luxembourg: IEEE STANDARD, 758-1979 IEEE Standard Subroutines for
Office Central de Vente des Publications des Communautes Eu- Computer Automated Measurement and Control (CAMAC),
ropeennes, 1972. IEEE, 1979.
Coaxial Cable Connectors Used in Nuclear Instrumentation, In- SAGNELL, L., CERN 19 Inch Chassis Systems, CERN Report 62-
ternational Electrotechnical Commission Publication 313, 1st. 29, Geneva, Switzerland: European Organization Nuclear Re-
Ed., Geneva, Switzerland: International Electrotechnical Com- search, 1962.
mission, 1969.
Standard Nuclear Instrument Modules, U.S. AEC Report TID-
COSTRELL, L., “NIM Standard,” in Instrumentation in Applied 20893, Washington DC: U.S. Gov. Printing Office, 1964; super-
Nuclear Chemistry, Ch. 5, J. Kruger, Ed., New York: Plenum seded in 1974 by TID-20893, Rev. 4.
Press, 1973.
Standard NIM Instrumentation System, U.S. DOE Report
DOE/ER-0457T, Standard NIM Instrumentation System, U.S. ER/DOE-0457T, Washington, DC: U.S. Department of Energy,
NIM Committee, US DOE, 1990. 1990.
ESONE System of Nuclear Electronics, European Atomic Energy United Kingdom Atomic Energy Authority Specifications and
Community, EURATOM, Report EUR 1831e, Luxembourg: Of- Guide to the 2000 Series Unit-Equipment, AERE(R) 11048,
fice Central de Vente des Publications des Communautes Eu- Berkshire, England: U.K. Atomic Energy Research Establish-
ropeennes, 1964. ment, Harwell, 1962.
IEEE STANDARD, 583-1982 IEEE Standard Modular Instrumen- Why 50 Ohms?, Microwaves 101, Online encyclopedia, 2009-01-
tation and Digital Interface System (CAMAC), IEEE, 1982. 13; Retrieved 2013-04-10.
IEEE STANDARD, 595-1982 IEEE Standard Serial Highway In- Coax Power Handling, Microwaves 101, Online encyclopedia,
terface System (CAMAC), IEEE, 1982. 2009-01-13; Retrieved 2013-04-10.
Chapter 3

Basic Atomic and Nuclear Physics

I claim that relativity and the rest of modern physics is not complicated. It can be explained
very simply. It is only unusual or, put another way, it is contrary to common sense.
Edward Teller

The main topic of this book is radiation detection and measurement; however, in order to understand the
principles involved in this discipline it is necessary to comprehend the basic ideas of modern physics upon
which these principles are based. It is not the intent in this and the next few chapters to present a detailed
derivation of the many topics addressed by atomic and nuclear physics. Rather, several topics important
for radiation detection are reviewed. Such a review does not go into great detail about the derivation of the
results, mainly because there are many excellent and thorough treatments already published such as books
by Kaplan [1962], Evans [1955], and Griffiths [2004, 2005]. It should also be noted that much of the material
in this and the next chapter have been extracted from Shultis and Faw [2008].
In this chapter, the important concepts of special relativity, wave-particle duality, and quantum mechanics
are reviewed. Then brief descriptions of the constituents of matter, atomic and nuclear models and the
energetics of nuclear interactions are provided. Finally, a review of radioactivity and its dynamics are
discussed.

3.1 Modern Physics Concepts


During the first three decades of the twentieth century, our understanding of the physical universe underwent
tremendous changes. Although the results of this revolution in physics are now called “modern” physics,
they are now almost a century old. Three of these modern physical concepts are (1) Einstein’s theory of
special relativity, which extended Newtonian mechanics; (2) wave-particle duality, which says that both elec-
tromagnetic waves and atomic particles have dual wave and particle properties; and (3) quantum mechanics,
which revealed that the microscopic atomic world is far different from our everyday macroscopic world. The
results and insights provided by these three advances in physics are fundamental to an understanding of
nuclear science and technology.

3.1.1 The Special Theory of Relativity


The classical laws of dynamics as developed by Newton were believed, for over 200 years, to describe all
motion in nature. Students still spend considerable effort mastering the use of these laws of motion. For
example, Newton’s second law, in the form originally stated by Newton, says the rate of change of a body’s

37
38 Basic Atomic and Nuclear Physics Chap. 3

momentum p equals the force F applied to it, i.e.,


dp d(mv)
F= = . (3.1)
dt dt
For a constant mass m, as assumed by Newton, this equation immediately reduces to the modern form of
the second law, F = ma, where a = dv/dt, the acceleration of the body.
In 1905 Einstein discovered that classical mechanics could not describe properly the behavior of an object
traveling near the speed of light and he found the necessary correction. In his theory of special relativity,1
Einstein showed that Eq. (3.1) is still correct, but that the mass of a body is not constant, but increases
with the body’s speed v. The form F = ma is thus incorrect. Specifically, Einstein showed that m varies
with the body’s speed as
mo
m=  , (3.2)
1 − v 2 /c2
where mo is the body’s “rest mass,” i.e., the body’s mass when it is at rest, and c is the speed of light
( 3 × 108 m/s). The validity of Einstein’s correction was immediately confirmed by observing that the
electron’s mass did indeed increase as its speed increased in precisely the manner predicted by Eq. (3.2).
Most fundamental changes in physics arise in response to experimental results that reveal an old theory
to be inadequate. However, Einstein’s correction to the laws of motion was produced theoretically before
being confirmed experimentally. This is perhaps not too surprising since in our everyday world the difference
between m and mo is incredibly small. For example, a satellite in a circular earth orbit of 7100 km radius
moves with a speed of 7.5 km/s. For this satellite the mass correction factor 1 − v 2 /c2 = 1 − 0.31 × 10−9 ,
i.e., relativistic effects change the satellite’s mass only in the ninth significant figure or by less than one part
in a billion! Thus for practical engineering problems in our macroscopic world, relativistic effects can safely
be ignored. However, at the atomic and nuclear level, these effects can be very important.

3.1.2 Principle of Relativity


The principle of relativity is older than Newton’s laws of motion. In Newton’s words (actually translated
from Latin) “The motions of bodies included in a given space are the same amongst themselves, whether
the space is at rest or moves uniformly forward in a straight line.” This means that experiments made in
a laboratory in uniform motion (e.g., in a non-accelerating train) produce the same results as when the
laboratory is at rest. Indeed, this principle of relativity is widely used to solve problems in mechanics by
shifting to moving frames of reference to simplify the equations of motion.
The relativity principle is a simple intuitive and appealing idea.
y y
But do all the laws of physics indeed remain the same in all non-
6 S 6 S accelerating (inertial ) coordinate systems? Consider the two coordi-
Ps
nate systems shown in Fig. 3.1. System S is at rest, while system S  is
(x, y, z, t)
   
moving uniformly to the right with speed v. At t = 0, the origin of S 
- (x , y , z , t ) is at the origin of S. The coordinates of some point P are (x, y, z) in
v
 S and (x , y  , z  ) in S  . Clearly, the primed and unprimed coordinates
-x x
are related by
Figure 3.1. Two inertial coordinate
systems. x = x − vt; y  = y; z  = z; and t = t. (3.3)

If these coordinate transformations are substituted into Newton’s laws of motion, the equations are
unchanged. For example, consider a force in the x-direction, Fx , acting on some mass m. Then the second

1 In 1915 Einstein published the general theory of relativity, in which he generalized his special theory to include gravitation.
Sec. 3.1. Modern Physics Concepts 39

law in the S  moving system is Fx = m d2 x /dt2 . Now transform this law to the stationary S system. For v
constant, one finds
d2 x d2 (x − vt) d2 x
Fx = m 2 = m = m .
dt d(t)2 dt2
Thus the second law has the same form in both systems. Since the laws of motion are the same in all inertial
coordinate systems, it follows that it is impossible to tell, from results of mechanical experiments, whether
or not the system is moving.
In the 1870s, Maxwell introduced his famous laws of electromagnetism. These laws explained all observed
behavior of electricity, magnetism, and light in a uniform system. However, when Eqs. (3.3) are used to
transform Maxwell’s equations to another inertial system, they assume a different form. Thus from optical
experiments in a moving system, one should be able to determine the speed of the system. For many
years Maxwell’s equations were thought to be somehow incorrect, but 20 years of research only continued to
reconfirm them. Eventually, some scientists began to wonder if the problem lay in the Galilean transformation
of Eqs. (3.3). Indeed, Lorentz observed in 1904 that if the transformation

x − vt t − vx/c2
x =  ; y  = y; z  = z; t =  (3.4)
1 − v 2 /c2 1 − v 2 /c2

is used, Maxwell’s equations become the same in all inertial coordinate systems. Poincaré, about this
time, even conjectured that all laws of physics should remain unchanged under the peculiar looking Lorentz
transformation. The Lorentz transformation is indeed strange, since it indicates that space and time are not
independent quantities. Time in the S  system, as measured by an observer in the S system, is different
from the time in the observer’s system.

3.1.3 Results of the Special Theory of Relativity


It was Einstein who, in 1905, showed that the Lorentz transformation was indeed the correct transformation
relating all inertial coordinate systems. He also showed how Newton’s laws of motion must be modified to
make them invariant under this transformation.
Einstein based his analysis on two postulates:
• The laws of physics are expressed by equations that have the same form in all coordinate systems
moving at constant velocities relative to each other.

• The speed of light in free space is the same for all observers and is independent of the relative velocity
between the source and the observer.

The first postulate is simply the principle of relativity, while the second states that light is observed to move
with speed c even if the light source is moving with respect to the observer. From these postulates, Einstein
demonstrated several amazing properties of our universe.
1. The laws of motion are correct, as stated by Newton, if the mass of an object is made a function of
the object’s speed v, i.e.,
mo
m(v) =  . (3.5)
1 − v 2 /c2
This result also shows that no material object can travel faster than the speed of light since the
relativistic mass m(v) must always be real. Further, an object with a rest mass (mo > 0) cannot even
travel at the speed of light; otherwise, its relativistic mass would become infinite and give it an infinite
kinetic energy.
40 Basic Atomic and Nuclear Physics Chap. 3

2. The length of a moving object in the direction of its motion appears smaller to an observer at rest,
namely, 
L = Lo 1 − v 2 /c2 . (3.6)
where Lo is the “proper length” or length of the object when at rest.
3. The passage of time appears to slow in a system moving with respect to a stationary observer. The
time t required for some physical phenomenon (e.g., the interval between two heart beats) in a moving
inertial system appears to be longer (dilated) than the time to for the same phenomenon to occur in
the stationary system. This phenomenon is called time dilation. The relation between t and to is
to
t=  . (3.7)
1 − v 2 /c2

4. Perhaps the most famous result from special relativity is the demonstration of the equivalence of mass
and energy by the well-known equation E = mc2 . By using Eqs. (3.1) and (3.2), Einstein showed that
the kinetic energy T of a particle is given by T = mc2 − mo c2 . Thus it is seen that the kinetic energy
is associated with the increase in the mass of the particle. Equivalently, this result can be written as
mc2 = mo c2 + T . The quantity mc2 can be interpreted as the particle’s “total energy” E, which equals
its rest-mass energy plus its kinetic energy. If the particle was also in some potential field, for example,
an electric field, the total energy would also include the potential energy. Thus it follows that

E = mc2 . (3.8)

This well-known equation is the cornerstone of nuclear energy analyses. It shows the equivalence of
energy and mass. One can be converted into the other in precisely the amount specified by E = mc2 .

The derivation of these important results can be found, for example, in Shultis and Faw [2008].
Relation Between Kinetic Energy and Momentum
Both classically and relativistically, the momentum p of a particle is given by

p = mv. (3.9)

In classical physics, a particle’s kinetic energy T is given by

mv 2 p2
T = = ,
2 2m
which yields √
p= 2mT . (3.10)
For relativistic particles, the relationship between momentum and kinetic energy is not as simple. Square
Eq. (3.5) to obtain
c2 − v 2
m2 = m2o ,
c2
or, upon rearrangement,
1
p2 ≡ (mv)2 = (mc)2 − (mo c)2 = [(mc2 )2 − (mo c2 )2 ].
c2
Sec. 3.2. Highlights in the Evolution of Atomic Theory 41

Because T = mc2 − mo c2 , the above result reduces to


1   1  
p2 = (T + mo c2 )2 − (mo c2 )2 = 2 T 2 + 2T moc2 . (3.11)
c2 c
Thus for relativistic particles
1 2
p= T + 2T mo c2 . (3.12)
c

Relativistic Particles
For most moving objects encountered in engineering analyses, the classical expression for kinetic energy can
be used. Only if an object has a speed near c must relativistic expressions be used. If the changeover from
classical to relativistic mechanics is associated with a specific relativistic mass increase, 0.1% for
 example,
the associated speed can be calculated from Eq. (3.5), which, for this example, yields 1.001 = 1/ 1 − v 2 /c2 .
Solving this result for v gives the relativistic speed threshold as v = 0.045c. Listed in Table 3.1 for several
important atomic particles are the rest mass energies and the kinetic energies required for a 0.1% mass
change.

Table 3.1. Rest mass energies and kinetic energies for a 0.1%
relativistic mass increase for four particles.

Particle rest mass kinetic energy for a


energy mo c2 0.1% increase in mass

electron 0.511 MeV 511 eV  0.5 keV


proton 938 MeV 938 keV  1 MeV
neutron 940 MeV 940 keV  1 MeV
α-particle 3751 MeV 3.8 MeV  4 MeV

3.2 Highlights in the Evolution of Atomic Theory


The concept of the atom is ancient. The Greek philosophers Leucippus and his pupil Democritus in the
fifth century BC conjectured that all matter was composed of indivisible particles or atoms (lit. “not to
be cut”). Unfortunately, Aristotle, whose ideas were more influential far into the Middle Ages, favored the
“fire, air, earth, and water” theory of Empedocles. According to the Roman poet Lucretius (100 B.C.), who
wrote at length about the nature of the universe in De Rerun Natura, the philosopher Epicurus (300 B.C.)
tried to revive the atomistic idea but little came from his effort because, of course, the idea was beyond any
experimental verification test at that time.
The modern concept of the atom had its origin in the observations of chemical properties made by eigh-
teenth and nineteenth century alchemists. Lavoisier first discovered that mass was conserved in chemical
reactions, and shortly after Gay-Lussac found that gases combined in simple ratios by volume. These obser-
vations prompted chemist Dalton in the period 1803–1808 to develop an explanation for the observations.
Dalton proposed his atomic hypothesis that stated: (1) each element consists of a large number of identical
particles (called atoms) that cannot be subdivided and that preserve their identity in chemical reactions; (2)
a compound’s mass equals the sum of the masses of the constituent atoms; and (3) chemical compounds are
formed by the combination of atoms of individual elements in simple proportions (e.g., 1:1, 1:2, etc.). This
atomic hypothesis explained chemical reactions and the distinct ratios in which elements combined to form
compounds. However, Dalton made no statement about the structure of an atom.
42 Basic Atomic and Nuclear Physics Chap. 3

At the beginning of the twentieth century, a wealth of experimental evidence allowed scientists to develop
ever more refined models of the atom, until our present model of the atom was essentially established
by the 1940s. The structure of the nucleus of an atom has now also been well developed qualitatively
and is supported by a wealth of nuclear data. However, work still continues on developing more refined
mathematical models to quantify the properties of nuclei and atoms.
In this section, a brief historical summary of the development of atomic models is presented. The
emphasis of the presentation is on the novel ideas that were developed, and little discussion is devoted to the
many experiments that provided the essential data for model development. Those interested in more detail,
especially about the seminal experiments, should refer to any modern physics text.

3.2.1 Radiation as Waves and Particles


For many phenomena, radiant energy can be considered as electromagnetic waves. Indeed Maxwell’s equa-
tions, which describe very accurately interactions of long wave-length radiation, readily yield a wave equation
for the electric and magnetic fields of radiant energy. Phenomena such as diffraction, interference, and other
related optical effects can be described only by a wave model for radiation.
However, near the beginning of the twentieth century, several experiments involving light and x rays
were performed that indicated that radiation also possessed particle-like properties. Today it is understood,
through quantum theory, that matter (e.g., electrons) and radiation (e.g., x rays) both have wave-like and
particle properties. This dichotomy, known as the wave-particle duality principle, is a cornerstone of modern
physics. For some phenomena, a wave description works best; for others, a particle model is appropriate.

3.2.2 Early Observations


In 1887, Heinrich Hertz observed that when ultraviolet light was illuminated upon one contact of a high
voltage circuit that an electric spark would issue a longer distance than when the contact was not exposed
to the light. J.J. Thomson demonstrated that the effect was caused by a negative charge being produced
on the contact surface by the ultraviolet light, referred to as the “photo-electric” effect. Later, in 1897,
J.J. Thomson correctly explained that cathode rays, which had been observed for decades, were actually
accelerated negative particles, which he referred to as “electrons”, as was correctly predicted by Benjamin
Franklin in 1746 with his Leyden jar experiments.2

3.2.3 The Photoelectric Effect


According to a classical (wave theory) description of light, the light energy was absorbed by the metal
surface, and when sufficient energy was absorbed to free a bound electron, a photoelectron would “boil” off
the surface. If light were truly a wave, one would expect the following observations:
• Photoelectrons should be produced by light of all frequencies.
• At low intensities, a time lag would be expected between the start of irradiation and the emission of a
photoelectron since it takes time for the surface to absorb sufficient energy to eject an electron.
• As the light intensity (i.e., wave amplitude) increases, more energy is absorbed per unit time and,
hence, the photoelectron emission rate should increase.
• The kinetic energy of the photoelectron should increase with the light intensity since more energy is
absorbed by the surface.

2 Franklinwas first to give the positive and negative designations to electricity, and he was the first to discover the principle
of conservation of charge. The cgs unit of electric charge was named after him, where one franklin (Fr) is equal to one
statcoulomb.
Sec. 3.2. Highlights in the Evolution of Atomic Theory 43

However, experimental results differed dramatically from these predictions. It was observed:
• For each metal there is a minimum light frequency below which no photoelectrons are emitted, no
matter how high the intensity.

• There is no time lag between the start of irradiation and the emission of photoelectrons, no matter
how low the intensity.

• The intensity of the light affects only the emission rate of photoelectrons.

• The kinetic energy of the photoelectron depends only on the frequency of the light and not on its
intensity. The higher the frequency, the more energetic is the photoelectron.

Einstein’s Explanation of the Photoelectric Effect


In 1905 Einstein introduced a new light model which explained all these observations.3 Einstein assumed
that light energy consists of photons or “quanta of energy,” each with an energy E = hν, where h is Planck’s
constant (6.626 × 10−34 J s) and ν is the light frequency. He further assumed that the energy associated
with each photon interacts as a whole, i.e., either all the energy is absorbed by an atom or none is. With
this “particle” model, the maximum kinetic energy of a photoelectron would be

E = hν − A, (3.13)

where A is the amount of energy (the so-called work function) required to free an electron from
the metal. Thus if hν < A, no photoelectrons are produced. Increasing the light intensity only
increases the number of photons hitting the metal surface per
unit time and, thus, the rate of photoelectron emission.
electrode
current Although Einstein was able to explain qualitatively the ob-
I meter served characteristics of the photoelectric effect, it was several
photoelectron
- years later before Einstein’s prediction of the maximum energy
V of a photoelectron, Eq. (3.13), was verified quantitatively using
light
the experiment shown schematically in Fig. 3.2. Photoelectrons
emitted from freshly polished metallic surfaces were absorbed
Figure 3.2. A schematic illustration of by a collector causing a current to flow between the collector
the experimental arrangement used to ver-
and the irradiated metallic surface. As an increasing negative
ify photoelectric effect.
voltage was applied to the collector, fewer photoelectrons had
sufficient kinetic energy to overcome this potential difference and the photoelectric current decreased to zero
at a critical voltage Vo at which no photoelectrons had sufficient kinetic energy to overcome the opposing
potential. At this voltage, the maximum kinetic energy of a photoelectron, Eq. (3.13), equals the potential
energy Vo qe the photoelectron must overcome, i.e.,

Vo qe = hν − A,

or
hν A
Vo = − , (3.14)
qe qe

3 Itis an interesting historical fact that Einstein received the Nobel prize for his photoelectric research and not for his theory
of relativity, which he produced in the same year.
44 Basic Atomic and Nuclear Physics Chap. 3

where qe is the electron charge (1.602 × 10−19 C).4 In 1912 Hughes showed that, for a given metallic surface,
Vo was a linear function of the light frequency ν. In 1916 Millikan, who had previously measured the electron
charge qe , verified that plots of Vo versus ν for different metallic surface had a slope of h/qe , from which
h could be evaluated. Millikan’s value of h was in excellent agreement with the value determined from
measurements of black-body radiation, in whose theoretical description Planck first introduced the constant
h.
The prediction by Einstein and its subsequent experimental verification clearly demonstrated the quantum
nature of radiant energy. Although the wave theory of light explained diffraction and interference phenomena,
scientists saw that the energy of electromagnetic radiation was in the form of individual quanta, each with
the same energy E = hν. A quantum of energy could then be transferred to a single atomic electron. This
quantization occurs no matter how weak the radiant energy.

3.2.4 Compton Scattering


Other experimental observations showed that light, besides having quantized energy characteristics, must
have another particle-like property, namely, momentum. According to the wave model of electromagnetic
radiation, radiation should be scattered from an electron with no change in wavelength. However, in 1922
Compton observed that x rays scattered from electrons had an increase in the wavelength Δλ = λ − λ
proportional to (1 − cos θs ) where θs was the scattering angle (see Fig. 3.3). To explain this observation, it
was necessary to treat x rays as particles with a linear momentum p = h/λ and energy E = hν = pc.

scattered
photon
λ 
H
Y  HH
θs pλ  HH pe
incident - r ?  HH
H  θs H
photon
λ HH 6φe 
φe HH
-
j
H
Hj pe
H pλ
recoil
electron

Figure 3.3. A photon with wavelength λ Figure 3.4. Conservation of momentum re-
is scattered by an electron. After scattering, quires the initial momentum of the photon pλ
the photon has a longer wavelength λ and equal the vector sum of the momenta of the
the electron recoils with an energy Te and scattered photon and recoil electron.
momentum pe .

In an x-ray scattering interaction, the energy and momentum before scattering must equal the energy
and momentum after scattering. Conservation of linear momentum requires the initial momentum of the
incident photon (the electron is assumed to be initially at rest) to equal the vector sum of the momenta of
the scattered photon and the recoil electron. This requires the momentum vector triangle of Fig. 3.4 to be

4 Historically,
the unit charge of an electron is denoted by ‘e’, which is also the SI symbol. Unfortunately, ‘e’ is also used as
Euler’s number   ∞

1 n 1
e = lim 1 + = .
n→∞ n n=0
n!
Hence, to avoid confusion the authors chose to designate the symbol qe as the magnitude for the unit charge 1.602 176 565 ×
10−19 coulombs.
Sec. 3.2. Highlights in the Evolution of Atomic Theory 45

closed, i.e.,
pλ = pλ + pe (3.15)
or from the law of cosines
pe2 = p2 + p2 − 2pλ pλ cos θs . (3.16)
λ λ
The conservation of energy requires
pλ c + me c2 = pλ c + mc2 (3.17)
where me is the rest-mass of the electron before the collision when it has negligible kinetic energy, and m is
its relativistic mass after scattering the photon. This result, combined with Eq. (3.11) (in which me ≡ mo ),
can be rewritten as
pλ + me c − pλ = pe2 + (me c)2 . (3.18)
Substitute for pe from Eq. (3.16) into Eq. (3.18), square the result, and simplify to obtain
1 1 1
− = (1 − cos θs ). (3.19)
pλ pλ me c
Because λ = h/p, this result gives the increase in the wavelength of the scattered electron as
h
λ − λ = (1 − cos θs ), (3.20)
me c
where h/(me c) = 2.431 × 10−6μm. Thus, Compton was able to predict the wavelength change of scattered x
rays by using a particle model for the x rays, a prediction which could not be obtained with a wave model.
This result can be expressed in terms of the incident and scattered photon energies, E and E  , respectively.
With the photon relations λ = c/ν and E = hν, Eq. (3.20) gives

1 1 1
− = (1 − cos θs ). (3.21)
E E m e c2

3.2.5 Electromagnetic Radiation: Wave-Particle Duality


Electromagnetic radiation assumes many forms encompassing radio waves, microwaves, visible light, x rays,
and gamma rays. Many properties are described by a wave model in which the wave travels at the speed of
light c and has a wavelength λ and frequency ν, which are related by the wave speed formula
c = λν. (3.22)
The wave properties account for many phenomena involving light such as diffraction and interference effects.
However, as Einstein and Compton showed, electromagnetic radiation also has particle-like properties,
namely, the light energy being carried by discrete quanta or packets of energy called photons. Each photon
has an energy E = hν and interacts with matter (atoms) in particle-like interactions (e.g., in the photoelectric
interactions described above).
Thus, light has both wave-like and particle-like properties. The properties or model to use depend on
the wavelength of the radiation being considered. If, for example, the electromagnetic radiation is visible
or infrared, radar or radio, with wavelengths upwards of ∼ 10−6 m and thus much greater than atom
dimensions, the wave model is usually most useful. However, if the electromagnetic radiation consists of
−8
ultraviolet, x rays or gamma rays, with wavelengths < ∼ 10 m or less, the corpuscular or photon model is
usually used. This is the model generally used throughout this book on radiation detection, because the
radiation of concern is usually penetrating short-wavelength electromagnetic radiation.
46 Basic Atomic and Nuclear Physics Chap. 3

incident N (θ)
electrons 6

 
* reflected
electrons
? ?θ
 *
 
B
  
t  AAt
At t t t -
 d - crystal plane 0 θ (deg) 90

Figure 3.5. Electrons scattering from atoms on a Figure 3.6. Observed number of
crystalline plane interfere constructively if the dis- electrons N (θ) scattered into a fixed
tance AB is a multiple of the electron’s de Broglie cone or directions about an angle θ
wavelength. by the atoms in a nickel crystal.

Photon Properties
Some particles must always be treated relativistically. For example, photons, by definition, travel with the
speed of light c. From Eq. (3.5), one might think that photons have an infinite relativistic mass, and hence,
from Eq. (3.12), infinite momentum. This is obviously not true since objects, when irradiated with light, are
not observed to jump violently. This apparent paradox can easily be resolved if the rest mass of the photon
is exactly zero, although its relativistic mass is finite. In fact, the total energy of a photon, E = hν, is due
strictly to its motion. Equation (3.12) immediately gives the momentum of a photon (with mo ≡ 0) as

E hν h
p= = = . (3.23)
c c λ
From Eq. (3.8), the photon’s relativistic mass is mc2 = E = hν or


m= . (3.24)
c2
3.2.6 Electron Scattering
In 1924 de Broglie postulated that, since light had particle properties, then for symmetry (physicists love
symmetry!), particles should have wave properties. Because photons had a discrete energy E = hν and mo-
mentum p = h/λ, de Broglie suggested that a particle, because of its momentum, should have an associated
wavelength λ = h/p.
Confirmation of Matter Waves
Davisson and Germer in 1927 confirmed that electrons did indeed behave like waves with de Broglie’s
predicted wavelength. In their experiment, shown schematically in Fig. 3.5, Davisson and Germer illuminated
the surface of a Ni crystal by a perpendicular beam of 54-eV electrons and measured the number of electrons
N (θ) reflected at different angles θ from the incident beam. According to the particle model, electrons should
be scattered by individual atoms isotropically and N (θ) should exhibit no structure. However, N (θ) was
observed to have a peak near 50◦ (see Fig. 3.6). This observation could only be explained by recognizing the
peak as a constructive interference peak — a wave phenomenon. Specifically, two reflected electron waves
are in phase (constructively interfere) if the difference in their path lengths AB in Fig. 3.5 is an integral
number of wavelengths, i.e., if d sin θ = nλ, n = 1, 2, . . . where d is the distance between atoms of the crystal.
In the following year, G.P. Thomson used a beam of more energetic electrons to pass through a thin foil
of a polycrystalline material. Film behind the foil clearly showed diffraction circles as a result of constructive
and destructive interference of the electron waves. In 1930 Estermann and Stern [1930] used a similar method
Sec. 3.3. Development of the Modern Atom Model 47

photographic
plate

a
b g

B out

vacuum

lead
radioactive
source

Figure 3.7. Deflection of α, β, and γ rays by a


magnetic field out of and perpendicular to the page.

to demonstrate that helium atoms also exhibit wave characteristics. These experiments and many similar
ones clearly demonstrated that electrons (and other particles such as atoms) have wave-like properties.

3.3 Development of the Modern Atom Model


In the first half of the twentieth century, the efforts to develop a model of an atom also provided additional
evidence that orbital electrons must have wave-like properties. In this section the historical development of
atomic models is reviewed.

3.3.1 Discovery of Radioactivity


In 1896, Becquerel discovered that uranium salts emitted rays similar to x rays in that they also fogged
photographic plates. Becquerel’s discovery was followed by isolation of two other radioactive elements,
radium and polonium, by the Curies in 1898. The radiation emission rate of radium was found to be more
than a million times that of uranium, for the same mass.
Experiments in magnetic fields showed that three types of radiation could be emitted from naturally
occurring radioactive materials. The identification of these radiations was made by the experimental ar-
rangement shown in Fig. 3.7. Radioactive material was placed in a lead enclosure and the emitted radiation
collimated in the upward direction by passing through the collimator. The entire chamber was evacuated
and a magnetic field was applied perpendicularly and directed outwardly from the plane of the page. With
this arrangement, Becquerel found three distinct spots at which radiation struck the photographic plate used
as a detector. The three different types of radiation, whose precise nature was then unknown, were called
alpha, beta, and gamma rays.
48 Basic Atomic and Nuclear Physics Chap. 3

- The beta rays, which were deflected to the left, were obviously
negatively charged particles, and were later found to be the same
as the “cathode” rays seen in gas discharge tubes. These rays were
identified by J.J. Thomson in 1898 as electrons. The gamma rays
were unaffected by the magnetic field and hence had to be un-
charged. Today, we know that gamma rays are high frequency elec-
tromagnetic radiation whose energy is carried by particles called
photons. The alpha particles, being deflected to the right, had pos-
+ itive charge. They were deflected far less than were the beta rays,
an indication that the alpha particles have a charge-to-mass ratio
qe /m far less than that of beta particles. Either the positive charge
of the alpha particle was far less than the negative charge of beta
particles and/or the alpha particle’s mass was far greater than that
thin of a beta particle.
glass
tube * a source A quantitative analysis of the deflection of alpha particles showed
that their speeds were of the order of 107 m/s. The charge-to-mass
vacuum
ratio was found to be 4.82 × 107 C kg−1 . By contrast, the charge-to-
mass ratio for the hydrogen ion is twice as large, namely, 9.59 × 107
C kg−1 . Thus, if the alpha particle had the same charge as the
hydrogen ion, its mass would have to be twice that of the hydrogen
mercury
ion. If the alpha particle were doubly charged, its mass would be
four times as large and would correspond to that of the helium atom.
That an alpha particle is an ionized helium atom was demonstrated
by Rutherford who used the experimental arrangement of Fig. 3.8.
Figure 3.8. Experimental arrange- The alpha particles from the radioactive source penetrate the thin-
ment used to identify the identity of α walled glass tube and are collected in the surrounding evacuated
particles. chamber. After slowing, the α particles capture ambient electrons
to form neutral helium atoms. The accumulated helium gas is then
compressed so that an electrical discharge occurs when a high voltage is applied between the electrodes. The
emission spectrum from the excited gas atoms was found to have the same wavelengths as that produced by
an ordinary helium-filled discharge tube. Therefore, the alpha particle must be a helium ion. The mass of
the alpha particle is four times the mass of hydrogen, but the charge on the alpha particle is only twice the
charge on a hydrogen ion.

3.3.2 Thomson’s Atomic Model: The Plum Pudding Model


The discovery of radioactivity by Becquerel in 1896 and Thomson’s discovery of the electron in 1898 provided
a basis for the first theories of atomic structure. In radioactive decay, atoms are transformed into different
atoms by emitting positively charged or negatively charged particles. This led to the view that atoms are
composed of positive and negative charges. If correct, the total negative charge in an atom must be an
integral multiple of the electronic charge and, since atoms are electrically neutral, the positive and negative
charges must be numerically equal.
The emission of electrons from atoms under widely varying conditions was convincing evidence that
electrons exist as such inside atoms. The first theories of atomic structure were based on the idea that atoms
were composed of electrons and positive charges. There was no particular assumption concerning the nature
of the positive charges because the properties of the positive charges from radioactive decay and from gas
discharge tubes did not have the qe /m consistency that was shown by the negative charges (electrons).
Sec. 3.3. Development of the Modern Atom Model 49

At the time of Thomson’s research on atoms, there was no information +

about the way that the positive and negative charges were distributed +
- + -
-
in the atom. Thomson proposed a model, simple but fairly accurate, + - +
+
considering the lack of information about atoms at that time. He - - +
-
assumed that an atom consisted of a sphere of positive charge of uni- + -
-
form density, throughout which was distributed an equal and opposite +

charge in the form of electrons. The atom was like a “plum pudding,”
with the negative charges dispersed like raisins or plums in a dough Figure 3.9. Thomson’s plum-
of positive electricity (see Fig. 3.9). The diameter of the sphere was pudding model of the atom.
of the order of 10−10 m, the magnitude found for the size of the atom.
This model explained three important experimental observations: (1) an ion is just an atom from which
electrons have been lost, (2) the charge on a singly ionized atom equals the negative of the charge of an
electron, and (3) the number of electrons in an atom approximately equals one-half of the atomic weight of
the atom, i.e., if the atom’s mass doubles, the number of electrons double.
Also it was known that the mass of the electron was known to be about one eighteen hundredth the mass
of the hydrogen atom. Therefore, the total mass of the electrons in an atom is a very small part of the total
mass of the atom, and, hence, practically all of the mass of an atom is associated with the positive charge
of the “pudding.”

3.3.3 The Rutherford Atomic Model


At the beginning of the twentieth century, Geiger and Marsden used alpha particles from a radioactive source
to irradiate a thin gold foil. According to the Thomson plum-pudding model, for a gold foil 4 × 10−5 cm in
thickness, the probability an alpha particle scatters at least by an angle φ was calculated to be exp(−φ/φm ),
where φm  1◦ . Thus, the probability that an alpha particle scatters by more than 90◦ should be about
10−40 . In fact, it was observed that one alpha particle in 8000 was scattered by more than 90◦ !
To explain these observations, Rutherford in 1911 concluded that the positively charged mass of an atom
must be concentrated within a sphere of radius about 10−12 cm. The electrons, therefore, must revolve
about a massive, small, positively charged nucleus in orbits with diameters of the size of atoms, namely,
about 10−8 cm. With such a model of the nucleus, the predicted deflection of alpha particles by the gold
foil fit the experimental data very well.

3.3.4 The Bohr Atomic Model


The Rutherford model of an atom was quickly found to have serious deficiencies. In particular, it violated
classical laws of electromagnetism. According to classical theory, an accelerating charge (the electrons in
circular orbits around a nucleus) should radiate away their kinetic energy within about 10−9 s and spiral
into the nucleus.5
But obviously atoms do not collapse. Were they to do so, the electromagnetic radiation emitted by the
collapsing electrons should be continuous in frequency, since as the electrons collapse, they should spiral ever
faster around the nucleus and hence experience increasing central accelerations. When atoms are excited by
an electrical discharge, for example, atoms are observed to emit light not in a continuous wavelength spectrum
but with very discrete wavelengths characteristic of the element. For example, part of the spectrum of light
emitted by hydrogen is shown in Fig. 3.10.

5 Thisradiation produced by an accelerated electric charge explains how radio waves are generated. Electrons are accelerated
back and forth along a wire (antenna) by an alternating potential with a well-defined frequency, namely that of the radio
waves that are emitted from the wire.
50 Basic Atomic and Nuclear Physics Chap. 3

n=3 4 5 6 7 ...

Ha Hb Hg Hd

o
6563.1 4861.3 4340.5 3646 A
red blue violet ultraviolet

Figure 3.10. Diagram of the lines of the Balmer series of atomic hydrogen. After
Kaplan [1963].

Table 3.2. Various hydrogen spectral series. It was found empirically that the wavelength of light
no Series name Spectrum location emitted by hydrogen (excited by electrical discharges)
1 Lyman ultraviolet could be described very accurately by the simple equa-
2 Balmer visible and near ultraviolet tion
3 Paschen infrared 1 1 1
= RH − 2 (3.25)
4 Brackett infrared λ n2o n
5 Pfund infrared
where no , n are positive integers with n > no and RH is
the Rydberg constant found empirically to have the value RH = 10 967 758 m−1 . The integer no defines a
series of spectral lines discovered by different researchers identified in Table 3.2.
The observed discrete-wavelength nature of light emitted by excited atoms was in direct conflict with
Rutherford’s model of the atom. In a series of papers published between 1913 and 1915, Bohr developed an
atomic model which predicted very closely the observed spectral measurements in hydrogen. Bohr visualized
an atom much like the Rutherford model with the electrons in orbits around a small dense central nucleus.
However, his model included several non-classical constraints. Bohr postulated:
1. An electron moves in a circular orbit about the nucleus obeying the laws of classical mechanics.
2. Instead of an infinity of orbits, only those orbits whose angular momentum L is an integral multiple
of h/2π are allowed.
3. Electrons radiate energy only when moving from one allowed orbit to another. The energy E = hν of
the emitted radiation is the difference between characteristic energies associated with the two orbits.
These characteristic energies are determined by a balance of centripetal and Coulombic forces.
Consider an electron of mass me moving with speed v in a circular orbit of radius r about a central
nucleus with charge Zqe . From postulate (1), the centripetal force on the electron must equal the Coulombic
attractive force, i.e.,
me v 2 Zqe2
= , (3.26)
r 4πo r2
where o is the permittivity of free space and qe is the charge of the electron. From postulate (2)
h
L ≡ me vr = n , n = 1, 2, 3, . . . . (3.27)

Solution of these relations for r and v yields

Zqe2 n2 h2  o
vn = and rn = , n = 1, 2, 3, . . . (3.28)
2o nh πme Zqe2
Sec. 3.3. Development of the Modern Atom Model 51

For n = 1 and Z = 1, these expressions yield r1 = 5.293 × 10−11 m and v1 = 2.187 × 106 m/s  c, indicating
that our use of non-relativistic mechanics is justified.
The electron has both potential energy6 Vn = −Zqe2 /(4πo rn ) and kinetic energy Tn = 12 me vn2 or, from
Eq. (3.26), Tn = 12 [Zqe2 /(4πo rn )]. Thus, the electron’s total energy En = Tn + Vn or, with Eq. (3.28),
   
1 Zqe2 Zqe2 1 Zqe2 me (Zq 2 )2
En = Tn + Vn = − =− = − 2 2 e2 . (3.29)
2 4πo rn 4πo rn 2 4πo rn 8o n h

For the ground state of hydrogen (n = 1 and Z = 1), this energy is E1 = −13.606 eV, which is the
experimentally measured ionization energy for hydrogen.
Finally, by postulate (3), the frequency of radiation emitted as an electron moves from an orbit with
“quantum number” n to an orbit denoted by no < n is given by

me Z 2 qe4 1 1
hνn→no = En − Eno = − 2 . (3.30)
82o h2 n2o n

Since 1/λ = ν/c, the wavelength of the emitted light is thus

1 me Z 2 qe4 1 1 1 1
= − 2 = R∞ 2 − 2 , n > no . (3.31)
λn→no 82o ch3 n2o n no n

Example 3.1: What is the energy (in eV) required to remove the electron in the ground state from singly
ionized helium?

Solution:
For the helium nucleus Z = 2 and the energy of the ground state (n=1) is, from Eq. (3.29),

me (2qe2 )2
E1 = − .
82o h2

From Table A.1 in Appendix A, one finds h = 6.626×10−34 J s, me = 9.109×10−31 kg, qe = 1.6022×10−19 C,
and o = 8.854 × 10−12 F m−1 (= C2 J−1 m−1 ). Substitution of these values into the above expression for
E1 yields
 
−18 kg
E1 = −8.720 × 10 = −8.720 × 10−18 J
m−2 s2
= (−8.720 × 10−18 J)/(1.6022 × 10−19 J/eV) = −54.43 eV.

Thus, it takes 54.43 eV of energy to remove the electron from singly ionized helium.

Equation (3.31) has the same form as the empirical Eq. (3.25). However, in the present analysis it
has been implicitly assumed that the proton is infinitely heavy compared to the orbiting electron so that
the electron moves in a circular orbit about a stationary proton. The Rydberg constant in the above
result (with Z = 1) is thus denoted by R∞ , and is slightly different from RH for the hydrogen atom.
In reality, the proton and electron revolve about each other. To account for this, the electron mass in

6 The potential energy is negative because of the attractive Coulombic force, with energy required to extract the electron from
the atom. The zero reference for potential energy is associated with infinite orbital radius.
52 Basic Atomic and Nuclear Physics Chap. 3

Pfund series
n=6 n=7 (infrared)

n=5

Brackett series
n=4 (infrared)

n=3

n=2
Paschen series
(infrared)
n=1

Balmer series
(visible & near
ultraviolet)

0 1 nm
Lyman series
(ultraviolet)

Figure 3.11. Bohr orbits for the hydrogen atom showing the deexcitation transitions that are
responsible for the various spectral series observed experimentally. After Kaplan [1963].

Eq. (3.31) should be replaced by the electron’s reduced mass μe = me mp /(me + mp ) [Kaplan 1963]. This
is a small correction since μe = 0.999445568 me, nevertheless an important one. With this correction,
RH = μe qe4 /(82o ch3 ) = 10 967 758 m−1 , which agrees with the observed value to eight significant figures!
The innermost orbits of the electron in the hydrogen atom are shown schematically in Fig. 3.11 to scale.
The electronic transitions that give rise to the various emission series of spectral lines are also shown. The
Bohr model, with its excellent predictive ability, quantizes the allowed electron orbits. Each allowed orbit is
defined by the quantum number n introduced through Bohr’s second postulate, a postulate whose justification
is that the resulting predicted emission spectrum for hydrogen is in amazing agreement with the observation.

3.3.5 Extension of the Bohr Theory: Elliptic Orbits


The Bohr theory was very successful in predicting with great accuracy the wavelengths of the spectral lines
in hydrogen and singly ionized helium. Shortly after Bohr published his model of the atom, there was a
significant improvement in spectroscopic resolution. Refined spectroscopic analysis showed that the spectral
lines were not simple, but consisted of a number of lines very close together, a so-called fine structure. In
terms of energy levels, the existence of a fine structure means that instead of a single electron energy level for
each quantum number n, there are actually a number of energy levels lying close to one another. Sommerfeld
partly succeeded in explaining some of the lines in hydrogen and singly ionized helium by postulating elliptic
orbits as well as circular orbits (see Fig. 3.12). These elliptical orbits required the introduction of another
quantum number to describe the angular momentum of orbits with varying eccentricities.
Sommerfeld showed that, in the case of a one-electron atom, the fine structure could be partially explained.
When the predictions of Sommerfeld’s model were compared to experimental results on the resolution of the
Balmer lines for He+ , the theory predicted more lines than were observed in the fine structure. Agreement
Sec. 3.3. Development of the Modern Atom Model 53

n=1
n=2
n=3
n=4
Figure 3.12. Relative positions and dimensions of the elliptical orbits cor-
responding to the first four values of the quantum number n in Sommerfeld’s
modification for the hydrogen atom. After Kaplan [1963].

between theory and experiment required the new quantum number to be constrained by an empirical or
ad hoc selection rule which limited the number of allowed elliptical orbits and the transitions between the
orbits.
For two-electron atoms, difficulties arose in the further refinement of Bohr’s theory. To account for the
observed splitting of the spectral lines in an applied magnetic field, it was necessary to introduce a third
quantum number m, related to the orientation of the elliptical orbits in space. In the presence of a magnetic
field, there is a component of the angular momentum in the direction of the field. This modification again
led to the prediction of more spectral lines than were experimentally observed, and a second set of selection
rules had to be empirically introduced to limit the number of lines.
Further difficulties arose when the model was applied to the spectrum of more complicated atoms. In
the spectra of more complicated atoms, multiplet structure is observed. Multiplets differ from fine structure
lines in that lines of a multiplet can be widely separated. The lines of sodium with wavelengths of 589.593
nm and 588.996 nm are an example of a doublet. Triplets are observed in the spectrum of magnesium.
These difficulties (and others) could not be resolved by further changes of the Bohr theory. It became
apparent that these difficulties were intrinsic to the model. An entirely different approach was necessary to
solve the problem of the structure of the atom and to avoid the need to introduce empirical selection rules.

3.3.6 The Quantum Mechanical Model of the Atom


From the ad hoc nature of quantum numbers and their selection rules used in refinements of the basic Bohr
model of the atom, it was apparent an entirely different approach was needed to explain the details of
atomic spectra. This new approach was introduced in 1925 by Schrödinger who brought wave or quantum
mechanics to the world. Here, only a brief summary is given. Schrödinger’s new theory (or model) showed
that there were indeed three quantum numbers (n, , m) analogous to the three used in the refined Bohr
models. Further, the values and constraints on these quantum numbers arose from the theory naturally—no
ad hoc selection rules were needed.
To explain the multiple fine-line structure in the observed optical spectra from atoms and the splitting of
some of these lines in a strong magnetic field (the anomalous Zeeman effect), the need for a fourth quantum
number ms was needed. This quantum number accounted for the inherent angular momentum of the electron
equal to ±h/2π. In 1928, Dirac showed that this fourth quantum number also arises from the wave equation
if it is corrected for relativistic effects.
In the quantum mechanical model of the atom, the electrons are no longer point particles revolving
around the central nucleus in orbits. Rather, each electron is visualized as a standing wave around the
nucleus. The amplitude of this wave (called a wave function) at any particular position gives the probability
that the electron is in that region of space. Example plots of these wave functions for the hydrogen atom
are given in Fig. 3.16. Each electron wave function has a well-defined energy which is specified uniquely by
the four quantum numbers defining the wave function.
54 Basic Atomic and Nuclear Physics Chap. 3

3.3.7 Wave-Particle Duality


The fact that particles can behave like waves and that electromagnetic waves can behave like particles seems
like a paradox. What really is a photon or an electron? Are they waves or particles? The answer is that
entities in nature are more complex than is often thought, and they have, simultaneously, both particle
and wave properties. Which properties dominate depends on the object’s energy and mass. The de Broglie
wavelength is given by
h hc
λ= = √ 2 (3.32)
p T + 2T mo c2

For a classical object (T 2  2T moc2 ), the wavelength is given by λ = h/ 2mo T . However, as the object’s
speed increases, its behavior eventually becomes relativistic (T 2mo c2 ) and the wavelength varies as
λ = hc/T , the same as that for a photon. When the wavelength of an object is much less than atomic
dimensions (∼ 10−10 m), it behaves more like a classical particle than a wave. However, for objects with
longer wavelengths, wave properties tend to be more apparent than particle properties.

3.4 Quantum Mechanics


The demonstration that particles (point objects) also had wave properties led to another major advance of
modern physics. Because a material object such as an electron has wave properties, it should obey some
sort of wave equation. Indeed, Schrödinger in 1925 showed that atomic electrons could be well described
as standing waves around the nucleus. Further, the electron associated with each wave could have only
a discrete energy. The branch of physics devoted to this wave description of particles is called quantum
mechanics or wave mechanics.

3.4.1 Schrödinger’s Wave Equation


To illustrate Schrödinger’s wave equation, consider an analogy to the standing waves produced by a plucked
string of length L anchored at both ends. The wave equation that describes the displacement Ψ(x, t) as a
function of position x from one end of the string, which has length L, and at time t is [Riley et al. 2006]

∂ 2 Ψ(x, t) 1 ∂ 2 Ψ(x, t)
2
= 2 . (3.33)
∂x u ∂t2
Here u is the wave speed. There are infinitely many discrete solutions to this homogeneous partial differential
equation, subject to the boundary condition Ψ(0, t) = Ψ(L, t) = 0, namely,
 
nπx nπut
Ψ(x, t) = A sin sin , n = 1, 2, 3 . . . (3.34)
L L

That this is the general solution can be verified by substitution of Eq. (3.34) into Eq. (3.33). The frequencies
ν of the solutions are also discrete. The time for one cycle is tc = 1/ν so that nπutc /L = 2π; thus
nu
ν= , n = 1, 2, 3, . . . .
2L
Notice that the solution of the wave equation Eq. (3.34) is separable, i.e., it has the form Ψ(x, t) =
ψ(x)T (t) = ψ(x) sin(2πνt). Substitution of this separable form into Eq. (3.33) yields

d2 ψ(x) 4π 2 ν 2
+ ψ(x) = 0
dx2 u2
Sec. 3.4. Quantum Mechanics 55

or, since u = λν,


d2 ψ(x) 4π 2
+ 2 ψ(x) = 0. (3.35)
dx2 λ
To generalize to three-dimensions, the operator d2 /dx2 is replaced by ∂ 2 /∂x2 + ∂ 2 /∂y 2 + ∂ 2 /∂z 2 ≡ ∇2 giving
4π 2
∇2 ψ(x, y, z) + ψ(x, y, z) = 0. (3.36)
λ2
Now apply this wave equation to an electron bound to an atomic nucleus. The positively charged nucleus
produces an electric field and an attractive electric force on the electron. The electron with (rest) mass m
has a total energy E, kinetic , and a potential energy U such that T = E −U . The wavelength of the
√ energy T 
electron is λ = h/p = h/ 2mT = h/ 2m(E − U ) (assuming the electron is non-relativistic). Substitution
for λ into Eq. (3.36) gives

2
− h2 ∇2 ψ(x, y, z) + U (x, y, z)ψ(x, y, z) = Eψ(x, y, z). (3.37)
8π m

This equation is known as the steady-state Schrödinger’s wave equation, and is the fundamental equation
of quantum mechanics. This is a homogeneous equation in which everything on the left-hand side is known
except, of course, ψ(x, y, z); but on the right-hand side the electron energy E is not known. Such an equation
generally has only the trivial null solution (ψ = 0); however, non-trivial solutions can be found if E has
very precise and discrete values7 E = En , n = 0, 1, 2, . . .. This equation then says that an electron around
a nucleus can have only very discrete values of E = En , a fact well verified by experiment. Moreover, the
wave solution of ψn (x, y, z) associated with a given energy level En describes the amplitude of the electron
wave. The interpretation of ψn is discussed below.

3.4.2 The Wave Function


The non-trivial solution ψn (x, y, z) of Eq. (3.37) when E = En (an eigenvalue of the equation) is called a
wave function. In general, this is a complex quantity which extends over all space, and may be thought of
as the relative amplitude of a wave associated with the particle described by Eq. (3.37). Further, because
Eq. (3.37) is a homogeneous equation, then, if ψ  is a solution, so is ψ = Aψ  , where A is an arbitrary
constant. It is usual to choose A so that the integral of ψψ ∗ = |ψ|2 over all space equals unity, i.e.,8

ψ(x, y, z)ψ ∗ (x, y, z) dV = 1. (3.38)

Just as the square of the amplitude of a classical wave defines the intensity of the wave, the square of
the amplitude of the wave function |ψ|2 gives the probability of finding the particle at any position in space.
Thus, the probability that the particle is in some small volume dV around the point (x, y, z) is

Prob = |ψ(x, y, z)|2 dV = ψ(x, y, z)ψ ∗ (x, y, z) dV.

From this interpretation of ψ, the normalization condition of Eq. (3.38) requires that the particle be some-
where in space.

7 Mathematicians call such an equation (subject to appropriate boundary conditions) an eigenvalue problem in which En is
called the eigenvalue and the corresponding solution ψn (x, y, z) the eigenfunction.
8 Here ψ ∗ denotes the complex conjugate of ψ.
56 Basic Atomic and Nuclear Physics Chap. 3

3.4.3 The Uncertainty Principle


With quantum/wave mechanics, it is no longer possible to say that a particle is at a particular location;
rather, one can say only that the particle has a probability ψψ ∗ dV of being in a volume dV . It is possible
to construct solutions to the wave equation such that ψψ ∗ is negligibly small except in a very small region
of space. Such a wave function thus localizes the particle to the very small region of space. However, such
localized wave packets spread out very quickly so that the subsequent path and momentum of the particle is
known only within very broad limits. This idea of there being uncertainty in a particle’s path and its speed
or momentum was first considered by Heisenberg in 1927.
If one attempts to measure both a particle’s position along the x-axis and its momentum, there will be an
uncertainty Δx in the measured position and an uncertainty Δp in the momentum. Heisenberg’s uncertainty
principle says there is a limit to how small these uncertainties can be, namely,
h
Δx Δp ≥ . (3.39)

This limitation is a direct consequence of the wave properties of a particle. The uncertainty principle can
be derived rigorously from Schrödinger’s wave equation; however, a more phenomenological approach is to
consider an attempt to measure the location of an electron with very high accuracy. Conceptually, one could
use an idealized microscope, which can focus very short wavelength light to resolve points that are about
10−11 m apart. To “see” the electron, a photon must scatter from it and enter the microscope. The more
accurately the position is to be determined (i.e., the smaller Δx), the smaller must be the light’s wavelength
(and the greater the photon’s energy and momentum). Consequently, the greater is the uncertainty in the
electron’s momentum Δp since a higher energy photon, upon rebounding from the electron, will change the
electron’s momentum even more. By observing a system, the system is necessarily altered.
The limitation on the accuracies with which both position and momentum (speed) can be known is an
important consideration only for systems of atomic dimensions. For example, to locate a mass of 1 g to
within 0.1 mm, the minimum uncertainty in the mass’s speed, as specified by Eq. (3.39), is about 10−26 m/s,
far smaller than errors introduced by practical instrumentation. However, at the atomic and nuclear levels,
the uncertainty principle provides a very severe restriction on how position and speed of a particle are
fundamentally intertwined.
There is a second uncertainty principle (also by Heisenberg) relating the uncertainty ΔE in a particle’s
energy E and the uncertainty in the time Δt at which the particle had the energy, namely,
h
ΔE Δt ≥ . (3.40)

This restriction on the accuracy of energy and time measurements is a consequence of the time-dependent
form of Schrödinger’s wave equation (not presented here), and is of practical importance only in the atomic
world. In the atomic and subatomic world involving transitions between different energy states, energy need
not be rigorously conserved during very short time intervals Δt, provided the amount of energy violation
ΔE is limited to ΔE  h/(2πΔt). This uncertainty principle is an important relation used to estimate the
lifetimes of excited nuclear states.

3.4.4 Particle in a Potential Well


To illustrate a solution of the Schrödinger’s wave equation, consider the case in which a particle is confined
within a one-dimensional potential well of finite depth and width a, as shown in Fig. 3.13. The potential is
constant at U (x) = 0 inside the well and is constant at a value labeled U0 for all regions outside the well. A
solution is sought for the three regions x < 0, 0 < x < a, and a < x. To simplify the analysis, it is common
to write Eq. (3.37) as
Sec. 3.4. Quantum Mechanics 57

U(x)

I II III
U0 ∇2 ψ(x, y, z) − 2m [U (x, y, z) − E]ψ(x, y, z) = 0, (3.41)
2

0 a where  ≡ h/(2π). Equation (3.41) can then be written for this one-
dimensional problem, under the the assumption that E < U0 , as
Figure 3.13. Finite square potential
well in which the particle energy is
d2 ψ(x)
less than the well potential. − k 2 ψ(x) = 0 for x < 0 or x > a, (3.42)
dX 2
and
d2 ψ(x)
+ φ2 α2 ψ(x) = 0 for 0 < x < a, (3.43)
dX 2
where k 2 ≡ 2mE/2 and φ2 ≡ 2m(U0 − E)/2 , both positive real numbers. From Eq. (3.42) one infers

ψ1 (x) = Aekx + Be−kx (x < 0) (3.44)

and
ψ3 (x) = F ekx + Ge−kx (x > a). (3.45)
The negative exponent term in region I and the positive exponent in region III must be excluded because
ψ(x) must not become infinite anywhere. Consequently, it is concluded that B = F = 0. From Eq. (3.43),
one has
ψ2 (x) = C sin(kx) + D cos(kx), (3.46)
the wave function in region II. A condition for the validity of Eq. (3.37) is that ∇2 ψ must exist and remain
finite everywhere. Here this condition requires ψ and dψ/dx be continuous across all boundaries (and at
infinity). From this requirement, values of the arbitrary constants A, G, C, and D can be determined.
Beforehand, a special case will be considered.
Particle in a Box
As U0 → ∞ the parameter φ → ∞ so that ψ1 (0) and ψ3 (a) must vanish so the only non-zero values of ψ(x)
are to be found in region II. In other words, the particle must be confined inside the well. From Eq. (3.46)
it is seen that
ψ2 (0) = 0 = D and ψ2 (x) = C sin(kx). (3.47)
Because ψ2 (a) = 0 = C sin(kx) to obtain non-trivial solutions the argument ka must assume discrete values
(or eigenvalues)

k= , n = ±1, ±2, ±3, . . . , . (3.48)
a
so the wavefunctions have the form
nπx
ψn (x) = C sin , (3.49)
a
and the energy of the particles is restricted to discrete values
 2
n2 h2 π 2 1 nπ
En = = . (3.50)
2m 2m a
58 Basic Atomic and Nuclear Physics Chap. 3

Because the energy of the particle is quantized, so is its momentum. Consequently,


p2n 2 kn2 n2 π 2 2
En = = = . (3.51)
2m 2m 2ma2
Finally the constant C is determined by the normalization condition
 ∞  a
nπx
ψn∗ (x)ψn (x) dx = A2n sin2 dx = 1. (3.52)
∞ 0 a

Upon evaluation of the integral, it is found An = 2/a so the wave functions for a particle in a box are

2 nπx
ψn (x) = sin . (3.53)
a a
In Fig. 3.14 the wave function is shown for n = 3.

Figure 3.14. The probability distribution for finding a particle in quantum


state n = 3 with energy E3 at points in a one-dimensional box.

From this analysis two distinct differences between classical mechanics and wave mechanics are apparent.
First, a particle confined to a box with rigid boundaries can have any speed, energy or linear momentum,
whereas in wave mechanics these variables have very distinct discrete values. Second, classically the particle
can be anywhere in the box with equal probability, whereas in wave mechanics the probability of observing
the particle varies with position.
Particle in a Finite Potential Well
Now let us return to a particle in a finite potential well. The most general solution is given by Eqs. (3.44),
(3.45), and (3.46), but now the boundary conditions are
ψ1 (−∞) = 0 , ψ3 (∞) = 0

ψ1 (0) = ψ2 (0) , ψ2 (a) = ψ3 (a)

dψ1  dψ2  dψ2  dψ3 


 =  ,  = 
dx x=0 dx x=0 dx x=a dx x=a
From the first two boundary conditions, the coefficients B and F must be zero if the wave function disappears
at ±∞. Hence, the wavefunctions reduce to
ψ1 (x) = Aeφx , ψ2 (x) = C sin(kx) + D cos(kx), ψ3 (x) = Ge−φx . (3.54)
Sec. 3.4. Quantum Mechanics 59

From the boundary conditions on ψ1 (0) and ψ3 (a) one finds A = D and φA = kC from which it follows that
D = kC/φ. Finally, the boundary conditions on the slope of the wave functions give

C sin(ka) + D cos(ka) = Ge−φa and k(C cos(ka) − D sin(ka)) = −φGe−φa . (3.55)

Substitution of D = kC/φ into Eqs. (3.55) yields

kC
C sin(ka) + cos(ka) = Ge−φa , (3.56)
φ
and  
k kC
( sin(ka) − C cos(ka) = Ge−φa . (3.57)
φ φ
Equating these two results and rearranging terms yields
 
C (k 2 − φ2 ) sin(ka) − 2φk cos(ka) = 0. (3.58)

Here it is assumed that the wavefunction ψ and coefficient C are non-zero. Equation (3.58) can then be
rewritten as
2φk
tan(ka) = 2 , (3.59)
k − φ2
a relation that relates the allowable values of φ and k. With the following substitutions,

2mU0 E  
φ0 = , ξ = , φ = φ0 1 − ξ, k = φ0 ξ, (3.60)
2 U0

Figure 3.15. Solutions to the finite square well for different values of φ0 α.
60 Basic Atomic and Nuclear Physics Chap. 3

Eq. (3.59) is reduced to the following



 2 ξ(1 − ξ)
tan(φ0 ξa) = . (3.61)
2ξ − 1
The solutions to Eq. (3.61) can be found by plotting both sides versus ξ and locating the intercepts, the
results of which are shown in Fig. 3.15. The allowed energies are found by multiplying the intercept value
of ξ by the potential energy U0 . The number of possible solutions, for a given value of φ0 a is seen to be
If (n − 1) π < φ0 a < nπ there are n solutions, n = 1, 2, 3, . . . .
Each solution defines an allowed energy state in the well. Observe from Fig. 3.15 that more states appear as
a is increased. Further, as a is decreased, the general trend is the solution for E (a function of ξ) increases
in value. In conclusion, (1) the number of allowed states increases as the well dimension a increases, and (2)
the allowed states are pushed upwards towards U0 as the well dimension a decreases.

3.4.5 The Hydrogen Atom


The hydrogen atom, the simplest atom, can be considered as a system of two interacting point charges, the
proton (nucleus) and an electron. The electrostatic attraction between the electron and proton is described
by Coulomb’s law. The potential energy of a bound electron is given by,
qe2
U (r) = − , (3.62)
r
where r is the distance between the electron and the proton.
The three-dimensional Schrödinger wave equation in spherical coordinates for the electron bound to the
proton is [Griffiths 2005]
   
1 ∂ 2 ∂ψ 1 ∂ ∂ψ 1 ∂ 2 ψ 8π 2 μ
2
r + 2
sin θ + 2 2 + 2 [E − U (r)] ψ = 0, (3.63)
r ∂r ∂r r sin θ ∂θ ∂θ r sin θ ∂φ2 h
where ψ = ψ(r, θ, φ) and μ is the electron mass (more correctly the reduced mass of the system).
To solve this partial differential equation for the wave function ψ(r, θ, φ), first replace it by three equivalent
ordinary differential equations involving functions of only a single independent variable. To this end, the
“separation of variables” method is used to seek a solution of the form
ψ(r, θ, φ) = R(r)Θ(θ)Φ(φ). (3.64)
Substitute this form into Eq. (3.63) and multiply the result by r2 sin2 θ/(RΘΦ) to obtain
   
sin2 θ d 2 dR(r) 1 d2 Φ(φ) sin θ d dΘ(θ) 8π 2 μ 2 2
r + + sin θ + r sin θ [E − U (r)] = 0. (3.65)
R(r) dr dr Φ(φ) dφ2 Θ(θ) dθ dθ h2
The second term is only a function of φ, while the other terms are independent of φ. This term, therefore,
must equal a constant, −m2 say. Thus,
d2 Φ(φ)
= −m2 Φ(φ). (3.66)
dφ2
Equation 3.65, upon division by sin2 θ and rearrangement becomes
   
1 d 2 dR(r) 8π 2 μr2 1 d dΘ(θ) m2
r + [E − U (r)] = − sin θ + = 0. (3.67)
R(r) dr dr h2 sin θΘ(θ) dθ dθ sin2 θ
Sec. 3.4. Quantum Mechanics 61

Since the terms on the left are functions only of r and the terms on the right are functions only of θ, both
sides of this equation must be equal to the same constant, β say. Thus two ordinary differential equations
are obtained, one for R(r) and one for Θ(θ), namely,
 
1 d dΘ(θ) m2
sin θ − Θ(θ) + βΘ(θ) = 0, (3.68)
sin θ dθ dθ sin2 θ
and
1 d 2 dR(r) β 8π 2 μ
r + R(r) + [E − U (r)] R(r) = 0. (3.69)
r2 dr dr r2 h2
Thus Eq. (3.63) is reduced to three ordinary, homogeneous, differential equations [Eq. (3.66), Eq. (3.68),
and Eq. (3.69)], whose solutions, when combined, give the entire wave function ψ(r, θ, φ) = R(r)Θ(θ)Φ(φ).
Each of these equations is an eigenvalue problem which yields “quantum numbers.” These quantum numbers
are used to describe the possible electron configurations in a hydrogen atom. The solutions also yield
relationships between the quantum numbers. The solution details are omitted—see any book on quantum
mechanics for the explicit solutions, for example Griffiths [2005]. The present discussion is restricted to the
essential features that arise from each equation.
The most general solution of Eq. (3.66) is

Φ(φ) = A sin mφ + B cos mφ, (3.70)

where A and B are arbitrary. However, it is required Φ(0) = Φ(2π) since φ = 0 and φ = 2π are the same
azimuthal angle. This boundary condition then requires m to be an integer, i.e., m = 0, ±1, ±2, . . .. For
each azimuthal quantum number m, the corresponding solution is denoted by Φm (φ).
Equation (3.68) in θ has normalizable solutions only if the separation constant has the form β = ( + 1)
where is a positive integer or zero, and is called the angular momentum quantum number. Moreover, the
azimuthal quantum number m must be restricted to 2 + 1 integer values, namely, m = 0, ±1, ±2, . . . , ± .
The corresponding solutions of Eq. (3.68) are denoted by Θm (θ) and are known to mathematicians as the
associate Legendre functions of the first kind; however, these details are not of concern here.
Finally, the solution of Eq. (3.69) for the radial component of the wave function, with β = ( + 1) and
U (r) = −qe2 /r, has normalizable solutions only if the electron’s energy has the (eigen)value

2π 2 μqe2
En = − , where n = 1, 2, 3, . . . (3.71)
h2 n2
The integer n is called the principal quantum number. Moreover, to obtain a solution, the angular quantum
number must be no greater than n − 1, i.e., = 0, 1, 2, . . . , (n − 1). The corresponding radial solution is
denoted by Rn (r) and mathematically is related to the associated Laguerre function.
Thus, the wave functions for the electron bound in the hydrogen atom have only very discrete forms
ψnm (r, θ, φ) = Rn (r)Θm (θ)Φm (φ). For the hydrogen atom, the energy of the electron is given by Eq. (3.71)
and is independent of the angular moment or azimuthal quantum numbers m and (this is not true for
multielectron atoms).
Special Notation for Electron States
A widely used, but strange, notation has been of long standing in describing the n and quantum numbers
of particular electron states. The letters s, p, d, f , g, h, and i are used to denote values of the angular
momentum quantum number of 0, 1, 2, 3, 4, 5, and 6, respectively. The value of n is then used as a prefix
to the angular moment letter. Thus a bound electron designated as 5f refers to an electron with n = 5 and
= 3.
62 Basic Atomic and Nuclear Physics Chap. 3

Examples of Wave Functions for Hydrogen



In Fig. 3.16, density plots of |ψnm |2 = ψnm ψnm are shown for different electron states in the hydrogen
atom. These plots are slices through the three-dimensional |ψ|2 in a plane perpendicular to the x-axis and
through the atom’s center. Because |ψ|2 is the probability of finding the electron in a unit volume, the
density plots directly show the regions where the electron is most likely to be found. The s states ( = 0) are
spherically symmetric about the nucleus, while all the others have azimuthal and/or polar angle dependence.
Electron Energy Levels in Hydrogen
For hydrogen, the energy of the bound electron is a function of n only (see Eq. (3.71)). Thus, for n > 1, the
quantum numbers and m may take various values without changing the electron energy, i.e., the allowed
electron configurations fall into sets in which all members of the set have the same energy. Thus, in Fig. 3.16,
an electron has the same energy in any of the four 4f electron states or the three 4d states, even though the
distribution of the electron wave function around the nucleus is quite different for each state. Such states
with the same electron binding energy are said to be degenerate.
The Spin Quantum Number
It was found, first from experiment and later by theory, that each quantum state (specified by values for
n, , and m) can accommodate an electron in either of two spin orientations. The electron, like the proton
and neutron, has an inherent angular momentum with a value of 12 h/(2π). In a bound state (defined by n,
, and m) the electron can have its spin “up” or “down” with respect to the z-axis used to define angular
momentum. Thus, a fourth quantum number ms = ± 12 is needed to unambiguously define each possible
electron configuration in an atom.
Dirac showed in 1928 that when the Schrödinger wave equation is rewritten to include relativistic effects,
the spin quantum number ms is inherent in the solution along with the quantum numbers n, , and m, which
were also inherent in the wave function solution of the non-relativistic Schrödinger’s wave equation [Schiff
1968].

3.4.6 Energy Levels for Multielectron Atoms


The solution of Schrödinger’s equation for the hydrogen atom can be obtained analytically, but the solution
for a multielectron system cannot. This difficulty arises because of the need to add a repulsive component
to the potential energy term to account for the interactions among the electrons. To obtain a solution for a
multielectron atom, numerical approximation techniques must be used together with high speed computers.
Such a discussion is far beyond the scope of this text.
There is, however, one important result for multielectron atoms that should be described here. The
energies of the electronic levels in atoms with more than one electron are functions of both n and . The
energy degeneracy in the angular momentum quantum number disappears. Thus states with the same n but
different values have slightly different energies, and there is a significant reordering of the electron energy
levels compared to those in the hydrogen atom.
Electron energy levels with the same value of n and but different values of m are still degenerate in
energy; however, this degeneracy is removed in the presence of a strong external magnetic field (the Zeeman
effect). An electron moving about a nucleus creates a magnetic dipole whose strength of interaction with an
external magnetic field varies with the quantum numbers and m.
The Electronic Structure of Atoms
Each electron in an atom can be characterized by its four quantum numbers n, , m, and ms . Further,
according to Pauli’s exclusion principle (1925), no two electrons in an atom can have the same quantum
numbers. An assignment of a set of four quantum numbers to each electron in an atom, no sets being alike
in all four numbers, then defines a quantum state for an atom as a whole. For ground-state atoms, the
1s 2p 3d 4f 2s 3p 4d 5f
Sec. 3.4. Quantum Mechanics

m=0 m = ±1 m = ±2 m = ±3 m=0 m = ±1 m = ±2 m = ±3

m=0 m = ±1 m = ±2 m=0 m = ±1 m = ±2

m=0 m = ±1 m=0 m = ±1

m=0 m=0

Figure 3.16. Density plots of ψ∗ ψ for different electron eigenstates in the hydrogen atom. Plots are sectional views of the probability density in a plane
containing the polar axis, which is vertical and in the plane of the paper. Scale of the right group is about 15% bigger than that of the left group. After:
R.B. Leighton, Principles of Modern Physics, McGraw Hill, New York, 1959.
63
64 Basic Atomic and Nuclear Physics Chap. 3

electrons are in the lowest energy electron states. For an atom in an excited state, one or more electrons are
in electron states with energies higher than some vacant states. Electrons in excited states generally drop
very rapidly (∼ 10−7 s) into vacant lower energy states. During these spontaneous transitions, the difference
in energy levels between the two states must be emitted as a photon (fluorescence or x rays) or be absorbed
by other electrons in the atom (thereby causing them to change their energy states).
Crucial to the chemistry of atoms is the arrangement of atomic electrons into various electron shells. All
electrons with the same n number constitute an electron shell. For n = 1, 2, . . . , 7, the shells are designated
K, L, M, . . . , Q.
Consider electrons with n = 1 (K shell). Since = 0 (s state electrons), then m = 0 and ms = ± 12 .
Hence, there are only 2 1s electrons, written as 1s2 , in the K shell. In the L shell (n = 2), = 0 or 1. For
= 0, there are two 2s electrons (denoted by 2s2 ), and for = 1 (m = −1, 0, 1), there are six 2p electrons
(denoted by 2p6 ). Thus in the L shell there are a total of eight electrons (2s2 2p6 ). Electrons with the same
value of (and n) are referred to as a subshell. For a given subshell, there are (2 + 1) m values, each with
two ms values, giving a total of 2(2 + 1) electrons per subshell, and 2n2 electrons per shell. A shell or
subshell containing the maximum number of electrons is said to be closed.
The Periodic Table of Elements can be described in terms of the possible number of electrons in the
various subshells. The number of electrons in an atom equals its atomic number Z and determines its
position in the Periodic Table. The chemical properties are determined by the number and arrangement of
the electrons. Each element in the table is formed by adding one electron to that of the preceding element
in the Periodic Table in such a way that the electron is most tightly bound to the atom. The arrangement
of the electrons for the elements with electrons in only the first four shells is shown in Table 3.3.

3.4.7 Success of Quantum Mechanics


Quantum mechanics has been an extremely powerful tool for describing the energy levels and the distributions
of atomic electrons around a nucleus. Each energy level and configuration is uniquely defined by four quantum
numbers: n the principal quantum number, the orbital angular momentum quantum number, m the z-
component of the angular momentum, and ms = ±1/2, the electron spin number. These numbers arise
naturally from the analytical solution of the wave equation (as modified by Dirac to include special relativity
effects) and thus avoid the ad hoc introduction of orbital quantum numbers required in earlier atomic models.
Inside the nucleus, quantum mechanics is also thought to govern. However, the nuclear forces holding the
neutrons and protons together are much more complicated than the electromagnetic forces binding electrons
to the nucleus. Consequently, much work continues in the application of quantum mechanics (and its
more general successor quantum electrodynamics) to predicting energy and configuration states of nucleons.
Nonetheless, the fact that electronic energy levels of an atom and nuclear excited states are discrete with very
specific configurations is a key concept in modern physics. Moreover, when one state changes spontaneously
to another state, energy is emitted or absorbed in specific discrete amounts.

3.5 The Fundamental Constituents of Ordinary Matter


Throughout this book, atoms, neutrons, and protons are treated as the only “fundamental” entities of
interest. Indeed, for the energies involved in practical nuclear and atomic interactions, this view is well
justified. However, at kinetic energies produced in particle accelerators or found in some cosmic rays, the
microscopic structure of matter is found to be much more complicated. This fine structure is not of practical
importance, however, in understanding radiation detectors; but for completeness, a brief overview of the
constituents of ordinary matter is presented here.
Although neutrons and protons are often considered “fundamental” particles, it is now known that they
are composed of other smaller particles called quarks held together by the exchange of massless particles
Sec. 3.5. The Fundamental Constituents of Ordinary Matter 65

Table 3.3. Electron shell arrangement for the lightest elements.

shell and electron designation


Element Z K L M N
1s 2s 2p 3s 3p 3d 4s 4p
H 1 1
He 2 2
Li 3 2 1
Be 4 2 2
B 5 2 2 1
C 6 2 2 2
N 7 2 2 3
O 8 2 2 4
F 9 2 2 5
Ne 10 2 2 6
Na 11 1
Mg 12 2
Al 13 2 1
Si 14 neon 2 2
P 15 configuration 2 3
S 16 2 4
Cl 17 2 5
Ar 18 2 6
K 19 1
Ca 20 2
Sc 21 1 2
Ti 22 2 2
V 23 3 2
Cr 24 5 1
Mn 25 5 2
Fe 26 6 2
Co 27 argon 7 2
Ni 28 configuration 8 2
Cu 29 10 1
Zn 30 10 2
Ga 31 10 2 1
Ge 32 10 2 2
As 33 10 2 3
Se 34 10 2 4
Br 35 10 2 5
Kr 36 10 2 6
Source: H.D. Bush, Atomic and Nuclear Physics, Prentice Hall,
Englewood Cliffs, NJ, 1962.
66 Basic Atomic and Nuclear Physics Chap. 3

called gluons, which are the carriers of the nuclear force. The protons and neutrons are bound together in a
nucleus by the residual interactions of the gluons in the neutrons and protons.
From studies of nuclear interactions produced by energetic cosmic rays and by particle accelerators, it is
believed that there are six different types or “flavors” of quarks with the fanciful names of up (u), down (d),
strange (s), charm (c), top (t), and bottom (b). For each quark there exists an antiquark, denoted by ū, d, ¯
etc. Each quark has a charge that is a fraction of the electron charge, namely the u, d, c, s, t, and b quarks
have charge 2/3, −1/3, 2/3, −1/3, 2/3, and −1/3, respectively. An antiquark has the same mass and angular
momentum, but opposite charge, as its real quark counterpart.
With the quarks and antiquarks two types of composite particles are formed. Baryons are composed of
3 quarks; for example, the neutron is a (ddu) composite (with a net charge of −1/3 − 1/3 + 2/3 = 0) and
the proton is a (uud) composite (with a net charge of 2/3 + 2/3 − 1/3 = 1). Mesons are composed of a
quark-antiquark pair; for example, a π+ meson is a (u,d) ¯ pair and a π − meson is a (ū,d) pair.
In addition to the quarks, there is another class of fundamental particles, called leptons consisting of
the electron, muon, and tau particles, each with an associated neutrino. Each of the leptons also has an
antiparticle. The quarks and leptons are exceedingly small with sizes less than about 10−19 m and are indeed
fundamental particles, i.e., not composite particles.
“Ordinary” matter is mostly composed of neutrons, protons, electrons, and neutrinos, each of which
has an angular momentum of ±h/(2π) (or a “spin” of 1/2) and, as such, are called fermions. Most of the
possible composite baryons and mesons are extremely unstable, with the heavier quarks decaying rapidly to
less massive ones by the forces mitigated by bosons, such as the photon or W ± boson, all of which have spin
= 1. For example, a free neutron can decay to a proton when a d quark changes to an u quark by emitting a
W − boson, which almost instantly decays to an electron (e− ) and an electron antineutrino (ν e ). The known
“fundamental” particles with their mass and charge are shown in Table 3.4. Whether there are additional
fundamental particles or even whether these particles are themselves composite particles made from even
more complex structures are unknown and are presently topics of great interest to high energy physicists.
However, in this work the electron, neutron, and proton are treated as fundamental indivisible particles,
because the composite nature of nucleons becomes apparent only under extreme conditions, such as those
encountered during the first second after the creation of the universe (the “big bang”) or in high energy
particle accelerators. Such gigantic energies are not addressed in this book. Rather, the energy of radiation
considered in this work is sufficient only to rearrange or remove the electrons in an atom or the neutrons
and protons in a nucleus.

3.5.1 Dark Matter and Energy


In our universe all ordinary matter is composed of electrons, neutrinos, and up and down quarks which are
bound together in protons and neutrons. However, over the past several decades, it has become apparent
that the gravitational forces from ordinary matter are insufficient to explain (1) the motion of stars near the
center of galaxies, (2) the filigreed distribution of galaxies in the universe, and (3) the accelerating expansion
of the universe itself. To explain these observations, astrophysicists have come to accept that there must be
vast amounts of dark matter to provide extra gravitational forces on stars in a galaxy and between galaxies.
Further, the amount of dark matter must be about five times that of ordinary matter. Although dark matter
can exert gravitational forces, it does not interact with light and, hence, is invisible to us. The fundamental
particles of dark matter are unknown and are the subject of much current speculation.
Astrophysicists have also had to postulate the existence of something called dark energy that must pervade
the universe in order to explain the observed accelerated expansion of our universe. Again, what constitutes
dark energy is unknown, but the amount of dark energy represents about 70% of the total mass/energy of
our universe!
Sec. 3.5. The Fundamental Constituents of Ordinary Matter 67

Table 3.4. The fundamental particles that make up “ordinary” matter. Each fermion has a
corresponding antiparticle with the same mass but of opposite charge. Data are from Yao et
al. [2006]

Fermions (spin = 1/2)

quarks leptons
mass mass
flavor charge (qe ) type charge (qe )
(GeV/c2 ) (GeV/c2 )
u 0.0015–0.0030 2/3 νe < 2 × 10−9 0
d 0.003–0.007 −1/3 e− 0.00051100 −1
c 1.25 2/3 νμ < 0.00019 0
s 0.095 ± 0.025 −1/3 μ− 0.10566 −1
t 176 2/3 ντ < 0.018 0
b 4.70 −1/3 τ− 1.7769 −1

Interaction Bosons (spin = 1)


mass
symbol force charge (qe )
(GeV/c2 )
gluon g strong 0 0
γ electromagnetic 0 0
W− weak 80.4 −1
W+ weak 80.4 1
Z0 weak 91.187 0
Higgs H explains mass 125 0

3.5.2 Atomic and Nuclear Nomenclature


The identity of an atom is uniquely specified by the number of neutrons N and protons Z in its nucleus. For
an electrically neutral atom, the number of electrons equals the number of protons Z, which is called the
atomic number. All atoms of the same element have the same atomic number. Thus, all oxygen atoms have
8 protons in the nucleus while all uranium atoms have 92 protons. The nucleus of an atom with a unique N
and A numbers is often referred to as a nuclide. There are about 3200 known nuclides.
However, atoms of the same element may have different numbers of neutrons in the nucleus. Atoms of
the same element, but with different numbers of neutrons, are called isotopes. The symbol used to denote a
particular isotope is
A
ZX

where X is the chemical symbol and A ≡ Z + N , which is called the mass number. For example, two
uranium isotopes are 235 238
92 U and 92 U. The use of both Z and X is redundant because one specifies the other.
Consequently, the subscript Z is often omitted, so that one may write, for example, simply 235 U and 238 U.9
Because isotopes of the same element have the same number and arrangement of electrons around the
nucleus, the chemical properties of such isotopes are nearly identical. Only for the lightest isotopes (e.g.,
hydrogen 1 H, deuterium 2 H, and tritium 3 H) are small differences observed. For example, light water 1 H2 O

9 To
avoid superscripts, which were hard to make on old-fashioned typewriters, the simpler form U-235 and U-238 was often
employed. However, with modern word processing, this form should no longer be used.
68 Basic Atomic and Nuclear Physics Chap. 3

freezes at 0◦ C, while heavy water 2 H2 O (or D2 O since deuterium is often given the chemical symbol D)
freezes at 3.82◦ C.

3.5.3 Relative Atomic Masses


The relative atomic mass A of any particular isotope, a dimensionless physical quantity, is the ratio of the
mass of one atom of the isotope to 1/12 the mass of an atom of 12 C. It is equivalent to the older term atomic
weight.10
The relative atomic mass of an element (typically composed of several isotopes) is slightly more involved.
The relative atomic mass of an element is ratio of the average mass of atoms in a sample of the element
to 1/12 the mass of an atom of 12 C. Thus the elemental relative atomic mass can vary depending on the
source of the sample. For example, elemental samples from different geological, biological, or extraterrestrial
sources often have different relative atomic masses because of their different isotopic compositions. In a
similar manner, the relative molecular weight is the average mass of molecules in a sample of the molecules
to 1/12 the mass of an atom of 12 C.
Most naturally occurring elements are composed of two or more isotopes. The isotopic abundance γi of
the i-th isotope in a given element is the fraction of the atoms in the element that are that isotope. As
with the elemental relative atomic mass, the isotopic abundances of a sample depends on the origins of the
sample. For a specified element, the elemental atomic weight is the weighted average of the atomic weights
of all naturally occurring isotopes of the element, weighted by the isotopic abundance of each isotope, i.e.,

 γi (%)
A= Ai , (3.72)
i
100

where the summation is over all the isotopic species comprising the element.
Both the terms relative atomic mass and atomic weight are often loosely used to refer to a standard
atomic weight. The elemental standard atomic weight is the average mass of the atoms in a normal sample
of the element to 1/12 the mass of an atom of 12 C. A normal sample is one from any reasonable source of
the element or its compounds used in commerce for industry and one that has not undergone significant
isotopic modification. These values are widely published in books and on wall charts of the Periodic Table.

3.5.4 The Atomic Mass Unit


Closely related to the concept of the relative atomic mass is the unified atomic mass unit,11 abbreviated
as u, defined such that the mass of a neutral atom of 12 C atom is 12 u. Equivalently, the mass of Avo-
gadro’s number of 12 C atoms (Avogadro’s number = 1 mole) is 0.012 kg. Thus, the SI unit for 1 u equals
(1/12)(0.012 kg/Na ) = 1.660 538 7 × 10−27 kg. An alternative and useful value of 1 u is 931.494 043/c2 MeV.
Masses of the different atomic nuclides are available in many compilations, e.g., Shultis and Faw [2008]. It
then follows that the mass M of an atom measured in atomic mass units numerically equals the atom’s
relative atomic mass A. The atomic weight of a nuclide almost equals (within less than one percent) the
atomic mass number A of the nuclide. Thus for approximate calculations, one can usually assume A  A.

10 The continued use of “atomic weight” and “relative atomic mass” has caused much controversy since the 1960s, primarily
because of the distinction in physics between “weight” and “mass.”
11 Previously called the atomic mass unit and abbreviated amu, it was based on 16 O rather than 12 C. This older metric and

terminology are obsolete. In terms of today, unified atomic mass unit and atomic mass unit are often casually interchanged,
but both refer to ‘u’ based on 12 C.
Sec. 3.5. The Fundamental Constituents of Ordinary Matter 69

3.5.5 Avogadro’s Number


Avogadro’s constant is the key to the atomic world since it relates the number of microscopic entities in a
sample to a macroscopic measure of the sample. Specifically, Avogadro’s constant Na  6.022 × 1023 equals
the number of atoms in 12 grams of 12 C. Few fundamental constants need be memorized, but an approximate
value of Avogadro’s constant should be.
The importance of Avogadro’s constant lies in the concept of the mole. A mole (abbreviated mol) of a
substance is defined to contain as many “elementary particles” as there are atoms in 12 g of 12 C. In older
texts, the mole was often called a “gram-mole” but is now called simply a mole. The “elementary particles”
can refer to any identifiable unit that can be unambiguously counted. One can, for example, speak of a mole
of stars, persons, molecules, or atoms.
Because the atomic weight of 12 C is defined to be 12 and because 12 g of 12 C is defined to contain 1 mol
of atoms, it follows that the mass in grams of any atomic species that numerically equals the dimensionless
atomic weight of the species must also contain 1 mole of atoms. The mass in grams of a substance that equals
the dimensionless atomic or molecular weight is sometimes called the gram atomic weight or gram molecular
weight. Thus, one gram atomic or molecular weight of any substance represents one mole of the substance and
contains as many atoms or molecules as there are atoms in one mole of 12 C, namely, Na atoms or molecules.
That one mole of any substance contains Na entities is known as Avogadro’s law and is the fundamental
principle that relates the microscopic world to the everyday macroscopic world. Table 3.5 illustrates how
Avogadro’s number Na , together with the atomic weight A, is the key to transforming between macroscopic
masses and the number of atoms.

Table 3.5. Use of Avogadro’s constant Na (atoms/mol) and the atomic


weight A (g/mol) to move between the atomic and macroscopic worlds.

Macroscopic Transformation Microscopic


←−
World −→ World
÷A m ×Na m
m (g) −→ (mols) −→ Na (atoms)
A A
N ×A N ÷Na
m= A (g) ←− (mols) ←− N (atoms)
Na Na
   
g ÷A ρ mol ×Na ρNa atoms
ρ −→ −→
cm3 A cm3 A cm3
A g ×A 1 ÷Na
m= ←− (mol) ←− 1 (atom)
Na atom Na

3.5.6 Mass of an Atom


With Avogadro’s number, many basic properties of atoms can be inferred. For example, the mass of an
individual atom can be found. Since a mole of a group of identical atoms (with a mass of A grams) contains
Na atoms, the mass of an individual atom is
M (g/atom) = A/Na  A/Na . (3.73)
The approximation of A by A is usually quite acceptable for all but the most precise calculations.

3.5.7 Number Density of Atoms and Isotopes


Avogadro’s number also determines the atom density (number of atoms per cm3 ) of a substance. For a
homogeneous substance of a single species and with mass density ρ g/cm3 , 1 cm3 contains ρ/A moles of the
70 Basic Atomic and Nuclear Physics Chap. 3

substance and ρNa /A atoms. The atom density N is thus

ρ
N (atoms/cm3 ) = Na . (3.74)
A

In radiation detection the number density of a particular isotope of an element is often of interest. To find
the atom density Ni of isotope i of an element with atom density N , simply multiply N by the fractional
isotopic abundance γi /100 for the isotope, i.e., Ni = (γi /100)N .
The same manner the atom density can be found of a particular element contained in a homogeneous
substance composed entirely of a certain molecule. In this case, N in Eq. (3.74) is the molecular density
and A the gram molecular weight. The number of atoms of a particular type, per unit volume, is found by
multiplying the molecular density by the number of the atoms of interest per molecule.
The composition of a mixture such as air is often specified by the mass fraction wi of each constituent.
If the mixture has a mass density ρ, the mass density of the ith constituent is ρi = wi ρ. The density Ni of
the ith component is thus
ρi N a wi ρNa
Ni = = . (3.75)
Ai Ai
If the composition of a substance is specified by a chemical formula, such as Xn Ym , the molecular weight
of the mixture is A = nAX + mAY and the mass fraction of component X is
nAX
wX = . (3.76)
nAX + mAY
Finally, as a general rule of thumb, it should be remembered that atom densities in solids and liquids are
usually between 1021 and 1023 atoms cm−3 . Gases at standard temperature and pressure are typically less
by a factor of 1000.

3.5.8 Size of an Atom


For a substance with an atom density of N atoms/cm3 , each atom has an associated volume of V = 1/N
cm3 . If this volume is considered a cube, the cube’s width is V 1/3 . For 238 U, the cubical size of an atom is
thus 1/N 1/3 = 2.7 × 10−8 cm. Measurements of the size of atoms reveal a diffuse electron cloud about the
nucleus. Although there is no sharp edge to an atom, an effective radius can be defined such that outside this
radius, an electron is very unlikely to be found. Almost all atoms with Z > 10 have radii between 1 × 10−8
and 2 × 10−8 cm. As Z increases, i.e., as more electrons and protons are added, the size of the electron cloud
changes little, but simply becomes more dense. Hydrogen, the lightest element, is also the smallest with a
radius of about 0.5 × 10−8 cm.

3.5.9 Nuclear Dimensions


Size of a Nucleus
If each proton and neutron in the nucleus has the same volume, the volume of a nucleus should be proportional
to A. This has been confirmed by many measurements that have explored the shape and size of nuclei.
Nuclei, to a first approximation, are spherical or very slightly ellipsoidal with a somewhat diffuse surface. In
particular, it is found that an effective spherical nuclear radius is
R = Ro A1/3 , with Ro  1.25 × 10−13 cm. (3.77)
The associated volume is
4 3
Vnucleus = πR  7.25 × 10−39 A cm3 . (3.78)
3
Sec. 3.6. Nuclear Reactions 71

Since the atomic radius of about 2 × 10−8 cm is 105 times greater than the nuclear radius, the nucleus
occupies only about 10−15 of the volume of an atom. If an atom were to be scaled to the size of a large
concert hall, then the nucleus would be the size of a very small gnat!
Nuclear Density
Since the mass of a nucleon (neutron or proton) is much greater than the mass of electrons in an atom
(mn  1837 me ), the mass density of a nucleus is

mnucleus A/Na
ρnucleus = = = 2.4 × 1014 g/cm3 .
Vnucleus (4/3)πR3

This is the density of the earth if it were compressed to a ball 200 m in radius.

3.6 Nuclear Reactions


Nuclear reactions play a very important role in many areas of nuclear science and engineering, because it is
through such reactions that various types of radiation are produced. The detection of such radiation is the
focus of this book. There are two main categories of nuclear reactions.
In the first category, the initial reactant X is a single atom or nucleus that spontaneously changes by
emitting one or more particles, i.e.,
X −→ Y1 + Y2 + · · · .
Such a reaction is called radioactive decay. Of the over 3200 known nuclides (an atom whose nucleus has a
unique number neutron and protons), all but 266 are radioactive. The variation in the number of radioactive
atoms over time and the different types of radioactive decay are addressed in the next section. Radioactive
decay is a particular type of nuclear reaction that, because it occurs spontaneously, must necessarily be
exothermic; i.e., mass must decrease in the decay process and energy must be emitted, usually in the form
of the kinetic energy of the reaction products.
The second broad category of nuclear reactions are binary reactions in which two nuclear particles (nu-
cleons, nuclei or photons) interact to form different nuclear particles.

X + x −→ Y1 + Y2 + · · · .

The most common types of such nuclear reactions are those in which some nucleon or nucleus x moves with
some kinetic energy and strikes and interacts with a nucleus X to form a pair of product nuclei y and Y ,
i.e.,
x + X −→ Y + y.
As a shorthand notation, such a reaction is often written as X(x, y)Y where x and y are usually the lightest
of the reaction pairs.

3.6.1 Q-Value for a Reaction


In any nuclear reaction, energy must be conserved, i.e., the total energy, including rest-mass energy, of the
initial particles must equal the total energy of the final products, i.e.,
 
[Ei + mi c2 ] = [Ei + mi c2 ] (3.79)
i i

where Ei (Ei ) is the kinetic energy of the ith initial (final) particle with a rest mass mi (mi ).
72 Basic Atomic and Nuclear Physics Chap. 3

Any change in the total kinetic energy of particles before and after the reaction must be accompanied by
an equivalent change in the total rest mass of the particles before and after the reaction. To quantify this
change in kinetic energy or rest-mass change in a reaction, a so-called Q-value is defined as

Q = (KE of final particles) − (KE of initial particles). (3.80)

Thus, the Q-value quantifies the amount of kinetic energy gained in a reaction. Equivalently, from Eq. (3.79),
this gain in kinetic energy must come from a decrease in the rest mass, i.e.,

Q = (rest mass of initial particles)c2 − (rest mass of final particles)c2 . (3.81)

The Q-value of a nuclear reaction may be either positive or negative. If the rest masses of the reactants
exceed the rest masses of the products, the Q-value of the reaction is positive with the decrease in rest mass
being converted into a gain in kinetic energy. Such a reaction is exothermic.
Conversely, if Q is negative, the reaction is endothermic. For this case, kinetic energy of the initial
particles is converted into rest-mass energy of the reaction products. The kinetic energy decrease equals the
rest-mass energy increase. Such reactions cannot occur unless the colliding particles have at least a certain
amount of kinetic energy.
Binary Reactions
For the binary reaction x + X → Y + y, the Q-value is given by

Q = (Ey + EY ) − (Ex + EX ) = [(mx + mX ) − (my + mY )]c2 . (3.82)

For most binary nuclear reactions, the number of protons is conserved so that the same number of electron
masses may be added to both sides of the reactions and, neglecting differences in electron binding energies,
the Q-value can be written in terms of atomic masses as

Q = (Ey + EY ) − (Ex + EX ) = [(Mx + MX ) − (My + MY )]c2 . (3.83)

Radioactive Decay Reactions


For a radioactive decay reaction X → Y + y, there is no particle x and the nucleus of X generally is at rest
so EX = 0. In this case
Q = (Ey + EY ) = [mX − (my + mY )]c2 > 0. (3.84)
Thus radioactive decay is always exothermic and the mass of the parent nucleus must always be greater than
the sum of the product masses. In some types of radioactive decay (e.g., beta decay and electron capture),
the number of protons is not conserved and care must be exercised in expressing the nuclear masses in terms
of atomic masses. This nuance is discussed in Section 3.6.3.

3.6.2 Conservation of Charge and the Calculation of Q-Values


In all nuclear reactions, total charge must be conserved. Sometimes this is not clear when writing the reaction
and subtle errors can be made when calculating the Q-value from Eq. (3.81). Consider, for example, the
reaction 168 O(n, p)167 N or
0 n + 8 O −→ 7 N + 1 p.
1 16 16 1
(3.85)
Sec. 3.7. Radioactivity 73

One might be tempted to calculate the Q-value as

Q = {mn + M (168 O) − M (167 N) − mp }c2 .

However, this is incorrect because the number of electrons is not conserved on both sides of the reaction.
On the left side there are 8 electrons around the 168 O nucleus, while on the right there are only 7 electrons in
the product atom 167 N. In reality, when the proton is ejected from the 168 O nucleus by the incident neutron,
an orbital electron is also lost from the resulting 167 N nucleus. Thus, the reaction of Eq. (3.85), to conserve
charge, should be written as
0 n + 8 O −→ 7 N + −1 e + 1 p.
1 16 16 0 1
(3.86)
The released electron can now be conceptually combined with the proton to form a neutral atom of 11 H, the
electron binding energy to the proton being negligible compared to the reaction energy. Thus, the reaction
can be approximated by
0 n + 8 O −→ 7 N + 1 H
1 16 16 1
(3.87)
and its Q-value is calculated as

Q = {mn + M (168 O) − M (167 N) − M (11 H)}c2 . (3.88)

In any nuclear reaction, in which the numbers of neutrons and protons are both conserved, the Q-value is
calculated by replacing any charged particle by its neutral-atom counterpart. Recall that 1 u is 931.494 043/c2
MeV, a value that readily allows reaction Q-values to be calculated in units of MeV when the atomic masses
are in atomic mass units.

3.6.3 Special Case for Changes in the Proton Number


The above procedure for calculating Q-values in terms of neutral-atom masses cannot be used when the
number of protons and neutrons are not conserved, and a more careful analysis is required. Such reactions
involve the so-called weak force that is responsible for changing neutrons into protons or vice versa. These
reactions are recognized by the presence of a neutrino ν (or antineutrino ν) as one of the reactants or products.
In such reactions, the conceptual addition of electrons to both sides of the reaction to form neutral atoms
often results in the appearance or disappearance of an extra free electron.

3.7 Radioactivity
Radioactive nuclei and their radiations have properties that are the basis of many of the ideas and techniques
of atomic and nuclear physics [Shultis and Faw 2008]. The spontaneous emission of alpha and beta particles
led to the concept that atoms are composed of smaller fundamental units. Likewise, the scattering of alpha
particles led to the idea of the nucleus, which is fundamental to the models used in atomic physics. The
discovery of isotopes resulted from the analysis of the chemical relationships among the various radioactive
elements. The bombardment of the nucleus by alpha particles caused the disintegration of nuclei and led to
the discovery of the neutron and the present model for the composition of the nucleus.
The discovery of artificial, or induced, radioactivity started a new line of nuclear research and hundreds
of artificial nuclei have been produced by many different nuclear reactions. The investigation of the emitted
radiations from radionuclides has shown the existence of nuclear energy levels similar to the electronic energy
levels. The identification and the classification of these levels are important sources of information about
the structure of the nucleus.
A number of radioactive nuclides occur naturally on the earth. One of the most important is 40 19 K, which
has an isotopic abundance of 0.0118% and a half-life of 1.28 × 109 y. Potassium is an essential element needed
74 Basic Atomic and Nuclear Physics Chap. 3

by plants and animals, and is an important source of human internal and external radiation exposure. Other
naturally occurring radionuclides are of cosmogenic origin. Tritium (31 H) and 146 C are produced by cosmic
ray interactions in the upper atmosphere, and also can cause measurable human exposures. 146 C (half-life
5730 y), which is the result of a neutron reaction with 147 N in the atmosphere, is incorporated into plants
by photosynthesis. By measuring the decay of 14 C in ancient plant material, the age of the material can be
determined.
Other sources of terrestrial radiation are uranium, thorium, and their radioactive progeny. All elements
with Z > 83 are radioactive. Uranium and thorium decay into daughter radionuclides, forming a series (or
chain) of radionuclides that ends with a stable isotope of lead or bismuth. There are four naturally occurring
radioactive decay series.
In all nuclear interactions, including radioactive decay, there are several quantities that are always con-
served or unchanged by the nuclear transmutation. The most important of these conservation laws include:
• Conservation of charge, i.e., the number of elementary positive and negative charges in the reactants
must be the same as in the products.
• Conservation of the number of nucleons, i.e., A is always constant. With the exception of EC and
β ± radioactive decay, in which a neutron (proton) transmutes into a proton (neutron), the number of
protons and neutrons is also generally conserved.
• Conservation of mass/energy (total energy). Although, neither rest mass nor kinetic energy is generally
conserved, the total (rest-mass energy equivalent plus kinetic energy) is conserved.
• Conservation of linear momentum. This quantity must be conserved in all inertial frames of reference.
• Conservation of angular momentum. The total angular momentum (or the spin) of the reacting particles
must always be conserved.

3.7.1 Types of Radioactive Decay


There are several types of spontaneous changes (or transmutations) that can occur in radioactive nuclides. In
each transmutation, the nucleus of the parent atom A Z P is altered in some manner and one or more particles
are emitted. If the number of protons in the nucleus is changed, then the number of orbital electrons in
the daughter atom D must subsequently also be changed, either by releasing an electron to or absorbing
an electron from the ambient medium. The most common types of radioactive decay are summarized in
Table 3.6.

3.7.2 Radioactive Decay Diagrams


Detailed descriptions of radioactive decay involve a considerable amount of information. One convenient
method for presenting such data is through a radioactive decay diagram. In Fig. 3.17 the hypothetical decay
of a radionuclide A
Z X is shown.
In a radioactive decay diagram, also sometimes called a nuclear-level diagram, the y-axis represents the
masses (or energy equivalents) of the nuclides involved and the x-axis shows the atomic number of the
nuclides. At the highest energy is the radionuclide of interest, the parent, whose ground state energy is
denoted by the bold horizontal line. The radioactive parent may decay in several ways to produce different
daughter nuclides. Decay that leads to daughters with lower atomic number than that of the parent have
daughter states shown to the left of the parent, with thin horizontal lines denoting excited states and a bold
line for the ground state. Daughters with increased atomic numbers are shown to the right of the parent.
Because all radioactive decays are exoergic, the mass of the daughter states must always be less than the
mass of the parent. Thus, the various decay modes (shown by descending arrows) always proceed from the
parent nuclide at the top of the diagram to daughter states below the parent, i.e., to states with less mass.
Sec. 3.7. Radioactivity 75

Table 3.6. Summary of important types of radioactive decay. The parent atom is denoted as P and the
product or daughter atom by D.

Decay Type Reaction Description


A ∗
gamma (γ) ZP −→ A
ZP +γ An excited nucleus decays to its
ground state by the emission of a
gamma photon.
alpha (α) A
ZP −→ A−4
Z−2 D +α An α particle is emitted leaving the
daughter with 2 fewer neutrons and
2 fewer protons than the parent.
negatron (β − ) A
ZP −→ Z+1
A
D+β − +ν A neutron in the nucleus changes to
a proton. An electron (β − ) and an
antineutrino (ν) are emitted.
positron (β + ) A
ZP −→ Z−1
A
D+β + +ν A proton in the nucleus changes into
a neutron. A positron (β + ) and a
neutrino (ν) are emitted.
− A ∗
Z P+e −→ Z−1 D +ν
A
electron An orbital electron is absorbed by the
capture (EC) nucleus, converts a nuclear proton into
a neutron and a neutrino (ν), and,
generally, leaves the nucleus in an
excited state.
proton (p) A
ZP −→ A−1
Z−1 D +p A nuclear proton is ejected from the
nucleus.
neutron (n) A
ZP −→ A−1
ZD +n A nuclear neutron is ejected from the
nucleus.
A ∗ −
internal con- ZP −→ [A +
Z P] + e The excitation energy of a nucleus is
version (IC) used to eject an orbital electron
(usually a K-shell electron).

The vertical energy/mass axis is on a relative scale for each daughter with zero energy being the ground
state of each daughter. The energy of each excited state is written on or adjacent to the horizontal line
representing the state. For an excited state with energy Ei above the ground state, the excited nucleus has
an excess mass Δmi = Ei /c2 greater than the mass of the nucleus in its ground state. Also often given is
the Q-value for the decay to the ground state. The Q-value for decay to an excited state is the Q-value to
the ground state less the nuclear excitation energy.

In the decay diagram of Fig. 3.17, the parent nucleus A Z X can decay to four different daughters: by β
A A−1 A
decay to Z+1 B, by neutron decay to Z X, by positron decay or electron capture to Z−1 C, and by α decay
to A−4
Z−2 D. For the alpha decay, note the break in the vertical line descending from the parent to indicate the
parent and daughters are on different energy/mass scales. Without such a break, the alpha decay daughter
would be far (almost 4 GeV) below the other decay daughters. Each decay arrow to a ground or excited state
is labeled by the type of decay, e.g., α1 , and the decay probability or frequency, e.g., f (α1 ). The frequency
fi , usually expressed in percent, gives the probability of that decay mode happening per decay of the parent.
Thus, all the decay frequencies should sum to 100%.
76 Basic Atomic and Nuclear Physics Chap. 3
A
ZX (T ½ )
parent

b -2 (fb2)
f a1)
a1 (
mass or energy equivalent

Am
) Z+1B (T½ )
(fa 2 E1
a
b-1 (fb )
2
E2 ) g (fg)
(fa 3
1
g3 (f g3) a3 n (fn) Q b-1
IC (f IC )

daughters
E1 Qn
g1 (f g1) g2 (fg2) g4 (f g4)
E3
+
Qa3 b (fb) E2 0
0 Qb+ g2 (fg2) A
A-4 Z+1B (stable)
Z-2 D (T½ ) E1
EC (fEC)
g3 (f g3) g1 (f g1)
A-1
ZX (T½ )
A
Z-1C (stable)

number of protons

Figure 3.17. A radioactive decay diagram showing four decay modes of the hypo-
thetical parent nuclide A
Z X in which four different daughter nuclides are produced.

Excited states of the daughter nucleus usually decay very rapidly to lower excited states or to the ground
state either by internal conversion, whereby the excitation energy is transferred to an orbital electron, or by
the emission of a photon called a gamma ray.12 The gamma ray energy is essentially equal to the difference
between the two energy states, because the kinetic energy of the recoiling atom is negligible. Thus, the
unique energies of gamma rays emitted in radioactive decay can be found readily from the energy levels in
the decay diagram.
Occasionally, an excited state can persist for an appreciable time. Such excited states are called metastable
and labeled as such with its half-life (see Section 3.7.5). For example, in Fig. 3.17, the first excited state
A Am
of the daughter Z+1 B is denoted as metastable by Z+1 B. This metastable state then decays to the ground
state by emission of a gamma ray or by internal conversion with the frequencies fγ and fIC , respectively.

3.7.3 Energetics of Radioactive Decay


In this section, the energies involved in the various types of radioactive decay are examined. Of particular
interest are the energies of the particles emitted in the decay process.13
Gamma Decay
97m Tc (90.5 d) In many nuclear reactions, a nuclide is produced whose nucleus is left in
43
96.56 keV an excited state. These excited nuclei usually decay very rapidly within
10−9 s to the ground state by emitting the excitation energy in the form
IC (99.7%) of a gamma ray. However, a few excited nuclei remain in an excited state
γ (0.31%) for a much longer time before they decay by gamma-ray emission. These
long-lived excited nuclei are called metastable nuclei or isomers. When
97 Tc
0 such an excited nuclide decays by gamma-ray emission, the decay is called
43 (2.6 x 106 y)
an isomeric transition. A simple example is shown in Fig. 3.18. The first
Figure 3.18. Radioactive decay excited state of 97m
43 Tc is a metastable state with a half-life of 90.5 d. It
diagram for the decay of 97m Tc. decays to the ground state with the emission of a 96.5 keV gamma photon.

12 Any photon emitted from a nucleus is termed a gamma photon. Photons emitted when atomic electrons change their energy
state are called x rays. Although x rays generally have lower energies than gamma photons, there are many exceptions.
13 From now on, kinetic energy is given the usual symbol E instead of T used up to now.
Sec. 3.7. Radioactivity 77

The gamma-decay reaction of an excited isotope of element P can be written as

A ∗
γ decay: ZP →A
ZP + γ . (3.89)

Energy conservation for this nuclear reaction requires



∗ 2
Z P )c ≡ M (Z P)c + E = M (Z P)c + EP + Eγ
M (A A 2 A 2
or E ∗ = EP + Eγ , (3.90)

where Eγ is the energy of the gamma photon, E ∗ is the excitation energy (above the ground state) of the
initial parent nucleus, and EP is the recoil kinetic energy of the resulting ground-state nuclide. If the initial
nuclide is at rest, the Q-value of this reaction is simply the sum of the kinetic energies of the products,
which, with Eq. (3.90), yields
Qγ = EP + Eγ = E ∗ . (3.91)
Linear momentum must also be conserved.14 Again with the parent at rest before the decay (i.e., with
zero initial linear momentum), the gamma photon and recoil nucleus must move in opposite directions and
have equal magnitudes of linear √momentum. Since the photon has momentum pγ = Eγ /c and the recoil
nuclide has momentum MP vP = 2MP EP , conservation of momentum requires
 Eγ2
Eγ /c = 2MP EP or EP = (3.92)
2MP c2
where MP ≡ M(A
Z P). Substitution of this result for EP into Eq. (3.91) yields
−1

Eγ = Qγ 1 +  Qγ = E ∗ . (3.93)
2MP c2
The approximation in this result follows from the fact that Eγ is at most 10–20 MeV, while 2MP c2 ≥ 4000
MeV. Thus, in gamma decay, the kinetic energy of the recoil nucleus is negligible compared to the energy of
the gamma photon and Eγ  Qγ = E ∗ .
Alpha-Particle Decay
From the prior discussion of nuclear structure, it was noted that nucleons tend to group themselves into
subunits of 42 He nuclei, often called alpha particles. Thus, it is not surprising that, for proton-rich heavy
nuclei, a possible mode of decay to a more stable state is by alpha-particle emission.
In alpha decay, the nucleus of the parent atom A Z P emits an alpha particle. The resulting nucleus of the
daughter atom A−4Z−2 D then has two fewer neutrons and two fewer protons. Initially, the daughter still has Z
electrons, two too many, and thus is a doubly negative ion [A−4
Z−2 D]
2−
, but these extra electrons quickly break
away from the atom, leaving it in a neutral state. The fast moving doubly charged alpha particle quickly loses
its kinetic energy by ionizing and exciting atoms along its path of travel and acquires two orbital electrons
to become a neutral 42 He atom. Since the atomic number of the daughter is different from that of the parent,
the daughter is a different chemical element. The alpha decay reaction is thus represented by

α decay: A
ZP −→ [A−4
Z−2 D]
2−
+ 42 α −→ A−4 4
Z−2 D + 2 He. (3.94)

14 Throughoutthis section, because of the comparatively large mass and low energy of the recoil atom, momentum of the recoil
is computed using laws of classical mechanics.
78 Basic Atomic and Nuclear Physics Chap. 3

Decay Energy Recall from the previous chapter, the Q-value of a nuclear reaction is defined as the decrease
in the rest mass energy (or increase in kinetic energy) of the product nuclei (see Eq. (3.81)). For radioactive
decay, the Q-value is sometimes called the disintegration energy. For alpha decay we have

Z P) − [M ([Z−2 D]
A−4
Qα /c2 = M(A 2−
) + m(42 α)]

 M(A
Z P) − [M(Z−2 D) + 2me + m(2 α)]
A−4 4

 M(A
Z P) − [M(Z−2 D) + M(2 He)].
A−4 4
(3.95)

In this reduction to atomic masses, the binding energies of the two electrons in the daughter ion and in the
He atom have been neglected since these are small (several eV) compared to the Q-value (several MeV). For
A−4
alpha decay to occur, Qα must be positive, or, equivalently, M(A 4
Z P) > M(Z−2 D) + M(2 He).

Kinetic Energies of the Products The disintegration energy Qα equals the kinetic energy of the decay
products. How this energy is divided between the daughter atom and the α particle is determined from the
conservation of momentum. The momentum of the parent nucleus was zero before the decay, and thus, from
the conservation of linear momentum, the total momentum of the products must also be zero. The alpha
particle and the daughter nucleus must, therefore, leave the reaction site in opposite directions with equal
magnitudes of their linear momentum to ensure the vector sum of their momenta is zero.
If we assume neither product particle is relativistic,15 conservation of energy requires

1 2 1
Qα = ED + Eα = MD vD + Mα vα2 , (3.96)
2 2
and conservation of linear momentum requires

MD vD = Mα vα , (3.97)

where MD ≡ M(A−4 Z−2 D) and Mα ≡ M(2 He). These two equations in the two unknowns vD and vα can be
4

solved to obtain the kinetic energies of the products. Solve Eq. (3.97) for vD and substitute the result into
Eq. (3.96) to obtain
1 Mα2 2 1 1 Mα
Qα = vα + Mα vα2 = Mα vα2 +1 . (3.98)
2 MD 2 2 MD
Hence, we find that the kinetic energy of the alpha particle is

MD AD
Eα = Qα  Qα . (3.99)
MD + Mα AD + Aα

Notice that, in alpha decay, the alpha particle is emitted with a well-defined energy. The recoiling nucleus
carries off the remainder of the available kinetic energy. From Eq. (3.96) we see ED = Qα − Eα , so that
from the above result
Mα Aα
ED = Qα  Qα . (3.100)
MD + Mα AD + Aα

15 Herea non-relativistic analysis is justified since the energy liberated in alpha decay is less than 10 MeV, whereas the rest mass
energy of an alpha particle is about 3727 MeV.
Sec. 3.7. Radioactivity 79

Alpha Decay Diagrams The above calculation assumes that the alpha decay proceeds from the
ground state of the parent nucleus to the ground state of the daughter nucleus. As dis-
cussed earlier, sometimes the daughter nucleus is left in an excited nuclear state (which ulti-
mately relaxes to the ground state by the emission of one or more gamma rays). In these
cases, the Qα -value of the decay is reduced by the excitation energy of the excited state.
226 Ra (1600y) Often a radionuclide that decays by alpha emission is ob-
88
served to emit alpha particles with several discrete energies.
0. 06 )
04 )
)
γ ( 00 7%

α1 (0.0003%)
00 1%
0%

This is an indication that the daughter nucleus is left in ex-


0. 02

α2 (0.0010%) cited states with nuclear masses greater than the ground state
γ ( .00

α3 (0.0065%)
0
γ(

635.5 mass by the mass equivalent of the excitation energy.


600.7 A simple case is shown in Fig. 3.19 for the decay of 226
88 Ra.
222
448.4 α4 (5.55%) This nuclide decays to the first excited state of 86 Rn 5.55%
γ (0.0054%) of the time and to the ground state 94.45% of the time. Two
α5 (94.44%) alpha particles with kinetic energies of Eα1 = 4.783 MeV
186.2 Qα5 = 4870.7 keV and Eα2 = 4.601 MeV are thus observed. Also a 0.186-MeV
γ (3.28%)
0 222 gamma ray is observed, with an energy equal to the energy
86Rn (3.824 d) difference between the two alpha particles or the two lowest
Figure 3.19. Energy levels for α decay of 226 Ra. nuclear states in 222
88 Rn.

Example 3.2: What is the initial kinetic energy of the alpha particle produced in the radioactive decay
226 222 4
88 Ra → 86 Rn + 2 He?

Solution:
The Qα value in mass units (i.e., the mass defect) is, from Eq. (3.95),
Qα = [M (226 222 4
88 Ra) − M ( 86 Rn) − M (2 He)]c
2

= [226.025402 − 222.017571 − 4.00260325]u × 931.5 MeV/u


= 0.005228 u × 931.5 MeV/u = 4.870 MeV.
The kinetic energy of the alpha particle from Eq. (3.99) is
AD 222
E α = Qα = 4.870 = 4.784 MeV.
AD + Aα 222 + 4
222
The remainder of the Qα energy is the kinetic energy of the product nucleus, 86 Rn, namely, 4.870 MeV −
4.783 MeV = 0.087 MeV.

Beta-Particle Decay
Many neutron-rich radioactive nuclides decay by changing a neutron in the parent (P) nucleus into a proton
and emitting an energetic electron. Many different names are applied to this decay process: electron decay,
beta minus decay, negatron decay, negative electron decay, negative beta decay, or simply beta decay. The
ejected electron is called a beta particle denoted by β − . The daughter atom, with one more proton in the
A
nucleus, initially lacks one orbital electron, and thus is a single charged positive ion, denoted by [Z−1 D]+ .
However, the daughter quickly acquires an extra orbital electron from the surrounding medium. The general
β − decay reaction is thus written as

β − decay: A
ZP −→ [Z+1
A
D]+ + 0
−1 e + ν e. (3.101)
80 Basic Atomic and Nuclear Physics Chap. 3

Here ν is an antineutrino, a chargeless particle with very little, if any, rest mass.16 That a third
product particle is involved with β − decay is implied from the observed energy and momentum of
the emitted β − particle. If the decay products were only the daughter nucleus and the β − particle,
then, as in α decay, conservation of energy and linear momentum would require that the decay en-
ergy be shared in very definite proportions between them. However, β − particles are observed to be
emitted with a continuous distribution of energies that has a
well-defined maximum energy (see Fig. 3.20). Rather than
abandon the laws of conservation of energy and momentum,
Pauli suggested in 1933 that at least three particles must be
produced in a β − decay. The vector sum of the linear momenta
of three products can be zero without any unique division of the
decay energy among them. In 1934 Fermi used Pauli’s sugges-
tion of a third neutral particle to produce a beta-decay theory
which explained well the observed beta-particle energy distri-
butions. This mysterious third particle, which Fermi named
the neutrino (lit. “little neutral one”), has since been verified
experimentally and today it is extensively studied by physi-
cists trying to develop fundamental theories of our universe.
The maximum energy of the β − spectrum corresponds to a
case in which the neutrino obtains zero kinetic energy, and the
Figure 3.20. Energy spectra of principle 38 Cl decay energy is divided between the daughter nucleus and the
β − particles. From Shultis and Faw [2000]. β − particle.
Decay Energy The beta decay energy is readily obtained from the Q-value of the decay reaction. Specifi-
cally,

Z P) − [M ([Z+1 D] ) + mβ − + mνe ]
Qβ − /c2 = M(A A +

 
Z P) − [ M(Z+1 D) − me + mβ − + mνe ] = M(Z P) − M(Z+1 D).
 M(A A A A
(3.102)
For β − decay to occur spontaneously, Qβ − must be positive or, equivalently, the mass of the parent atom
must exceed that of the daughter atom, i.e., M(A A
Z P) > M(Z+1 D).
38 Often in β − decay, the nucleus of the daughter is left in an
17Cl (37.24 min)
excited state. For example, 38 Cl decays both to the ground
state of the daughter 38 Ar as well as to two excited states
(see Fig. 3.21). The resulting β − energy spectrum (Fig. 3.20)
β1- (31.9%)
3810 keV is a composite of the β − particles emitted in the transition to
β-2 (10.5%) γ (31.9%) each energy level of the daughter. For a decay to an energy
2167 level E ∗ above the ground level, the mass of the daughter
β-3 (57.6%) γ (42.4%) atom in Eq. (3.102) M(Z+1 A
D) must be replaced by the mass
A ∗
Qβ3 = 4917
0
of the excited daughter M(Z+1 D )  M(Z+1 A
D)+E ∗ /c2 . Thus,
38
18 Ar (stable) Qβ − for β decay to an excited level with energy E ∗ above

ground level in the daughter is


Figure 3.21. Radioactive decay diagram for the
decay of 38 Cl. Three distinct groups of β − par- ∗ 2
Z P) − M(Z+1 D) − E /c .
Qβ − /c2 = M(A A
(3.103)
ticles are emitted.
16 The mass of the emitted neutrino is essentially that of the electron neutrino νe . The mass of νe is currently a subject of great
interest in the high-energy physics community. Recent experiments show that, if it has any mass, its mass is exceedingly small
and is less than a few eV mass equivalent (see Table 3.4). For the energetics of radioactive beta decay, the neutrino rest mass
is completely negligible and can be taken as zero.
Sec. 3.7. Radioactivity 81

Because the kinetic energy of the parent nucleus is zero, the Qβ − decay energy must be divided among
the kinetic energies of the products. The maximum kinetic energy of the β − particle occurs when the
antineutrino obtains negligible energy. In this case, since the mass of the β − particle is much less than that
of the daughter nucleus, Q = ED + Eβ −  Eβ − or

(Eβ − )max  Qβ − . (3.104)

Positron Decay
Nuclei that have too many protons for stability often decay by changing a proton into a neutron. In this
decay mechanism, an anti-electron or positron β + or +10 e, and a neutrino ν are emitted. The daughter atom,
with one less proton in the nucleus, initially has one too many orbital electrons, and thus is a negative ion,
denoted by [Z−1A
D]− . However, the daughter quickly releases the extra orbital electron to the surrounding
medium and becomes a neutral atom. The β + decay reaction is written as

β + decay: A
ZP −→ [Z−1
A
D]− + 0
+1 e + νe . (3.105)

The positron has the same physical properties as an electron, except that it has one unit of positive charge.
The positron β + is the antiparticle of the electron. The neutrino ν is required (as in β − decay) to conserve
energy and linear momentum since the β + particle is observed to be emitted with a continuous spectrum
of energies up to some maximum value (Eβ + )max . The neutrino ν in Eq. (3.105) is the antiparticle of the
antineutrino ν produced in beta-minus decay.
Decay Energy The decay energy is readily obtained from the Q-value of the decay reaction. Specifically,

Z P) − [M ([Z−1 D] ) + m(+1 e) + mνe ]
Qβ + /c2 = M(A A 0

 
Z P) − [ M(Z−1 D) + me + mβ + + mνe ]
 M(A A

Z P) − M(Z−1 D) − 2me
= M(A A
(3.106)

where the binding energy of the electron to the daughter ion and the neutrino mass have been neglected. If
the daughter nucleus is left in an excited state, the excitation energy E ∗ must also be included in the Qβ +
calculation, namely,
∗ 2
Z P) − M(Z−1 D) − 2me − E /c .
Qβ + /c2 = M(A A
(3.107)
∗ 2
Thus, for β + decay to occur spontaneously, Qβ + must be positive, i.e., M(A A
Z P) > M(Z−1 D) + 2me + E /c .
The maximum energy of the emitted positron occurs when the neutrino acquires negligible kinetic energy,
22
so that the Qβ + energy is shared by the daughter atom and the
11Na (2.602 y) positron. Because the daughter atom is so much more massive
β+ (89.84%) than the positron (by factors of thousands), almost all the Qβ +
EC (10.10%) energy is transferred as kinetic energy to the positron. Thus
1274 keV β+ (0.056%)
γ (99.94%)
Qβ+ = 1820 keV (Eβ + )max  Qβ + . (3.108)

0 An example of a radionuclide that decays by positron emis-


22
10Ne (stable) sion is 22
11 Na. The decay reaction is

Figure 3.22. Radioactive decay diagram for


positron emission from 22 Na.
22
11 Na −→ 22 +
10 Ne + β + νe ,
82 Basic Atomic and Nuclear Physics Chap. 3

and the level diagram for this decay is shown in Fig. 3.22. Notice that the daughter is almost always left in
its first excited state. This state decays, with a mean lifetime of 3.63 ps, by emitting a 1.274-MeV gamma
ray.
The emitted positron loses its kinetic energy by ionizing and exciting atomic electrons as it moves through
the surrounding medium. Eventually, it captures an ambient electron, forming for a brief instant a pseudo-
atom called positronium before they annihilate each other. Their entire rest mass energy 2me c2 is converted
into photon energy (the kinetic energy at the time of annihilation usually being negligible). Before the
annihilation, there is zero linear momentum, and there must be no net momentum remaining; thus, two
photons traveling in opposite directions must be created, each with energy E = me c2 = 0.511 MeV.
Electron Capture
In the quantum mechanical model of the atom, the orbital electrons have a finite (but small) probability of
spending some time inside the nucleus, the innermost K-shell electrons having the greatest probability. It is
possible for an orbital electron, while inside the nucleus, to be captured by a proton, which is thus transformed
into a neutron. Conceptually we can visualize this transformation of the proton as p + −10 e → n + ν, where
the neutrino is again needed to conserve energy and momentum. The general electron capture (EC) decay
reaction is written as

A ∗
EC decay: A
ZP −→ Z−1 D + νe . (3.109)

where the daughter is generally left in an excited nuclear state with energy E ∗ above ground level. Unlike in
most other types of radioactive decay, no charged particles are emitted. The only nuclear radiations emitted
are gamma photons produced when the excited nucleus of the daughter relaxes to its ground state. As the
outer electrons cascade down in energy to fill the inner shell vacancy, x rays and Auger electrons are also
emitted.
Decay Energy The decay energy is readily obtained from the Q-value of the decay reaction. If we assume
the daughter nucleus is left in its ground state

Z P) − [M(Z−1 D) + mνe ]
QEC /c2 = M(A A

 M(A
Z P) − M(Z−1 D).
A
(3.110)

If the daughter nucleus is left in an excited state, the excitation energy E ∗ must also be included in the QEC
calculation, namely,
∗ 2
QEC /c2 = M(A Z P) − M(Z−1 D) − E /c .
A
(3.111)
∗ 2
Thus, for EC decay to occur spontaneously, QEC must be positive, i.e., M(A A
Z P) > M(Z−1 D) + E /c .
+
Notice that both β and EC decay produce the same daughter nuclide. In fact, if the mass of the parent
is sufficiently large compared to the daughter, both decay modes can occur for the same radionuclide. From
Eq. (3.107) and Eq. (3.111), we see that if the parent’s atomic mass is not at least two electron masses
greater than the daughter’s mass, Qβ + is negative and β + decay cannot occur. However, QEC is positive as
long as the parent’s mass is even slightly greater than that of the daughter, and EC can still occur.
An example of a radionuclide that decays by electron capture is 74 Be. The decay reaction is
7
4 Be −→ 73 Li + νe .

The level diagram for this decay is shown in Fig. 3.23. Notice that in this example, the QEC of 862
keV is less than 2me c2 = 1022 keV so that there can be no competing β + decay. Finally, in an EC
Sec. 3.7. Radioactivity 83

7 transition, an orbital electron (usually from an inner shell)


4Be (53.29 d)
disappears leaving an inner electron vacancy. The remaining
EC (10.52%) atomic electrons cascade to lower orbital energy levels to fill
the vacancy, usually emitting x rays as they become more
477.6 keV EC (89.48%)
QEC = 861.8 keV tightly bound. The energy change in an electronic transition,
γ (10.52%) instead of being emitted as an x ray, may also be transferred
to an outer orbital electron ejecting it from the atom. These
0
7Li (stable) ejected electrons are called Auger electrons, named after their
3
discoverer, and appear in any process that leaves a vacancy
Figure 3.23. Decay of 7 Be by electron capture. in an inner electron shell.
Neutron Decay
A few neutron-rich nuclides decay by emitting a neutron producing a different isotope of the same parent
element. Generally, the daughter nucleus is left in an excited state which subsequently emits gamma photons
as it returns to its ground state. This decay reaction is


n decay: A
ZP −→ A−1 1
Z P + 0 n. (3.112)

An example of such a neutron decay reaction is 138 54 Xe → 54 Xe + n. Although, neutron decay is rare, it
137

plays a very important role in nuclear reactors. A small fraction of the radioactive atoms produced by fission
reactions decay by neutron emission at times up to minutes after the fission event in which they were created.
These neutrons contribute to the nuclear chain reaction and thus effectively slow it down, making it possible
to control nuclear reactors.
The Q-value for such a decay is
A−1 ∗ ∗ 2
Z P) − [M( Z P ) + mn ] = M(Z P) − M( Z D) − mn − E /c ,
A−1
Qn /c2 = M(A A
(3.113)

where E ∗ is the initial excitation energy of the daughter nucleus. Thus, for neutron decay to occur to even
A−1
the ground state of the daughter, M(A Z P) > M( Z D) + mn .

Proton Decay
A few proton-rich radionuclides decay by emission of a proton. In such decays, the daughter atom has an
extra electron (i.e., it is a singly charged negative ion). This extra electron is subsequently ejected from the
atom’s electron cloud to the surroundings and the daughter returns to an electrically neutral atom. The
proton decay reaction is thus

∗ −
p decay: A
ZP −→ [A−1 1
Z−1 D ] + 1 p. (3.114)

In this reaction P and D refer to atoms of the parent and daughter. Thus, the Q-value for this reaction is
A−1 ∗ −
 A−1 ∗ 
Qp /c2 = M(A Z P) − [M ([Z−1 D ] ) + mp ]  M(Z P) − [ M (Z−1 D ) + me + mp ]
A

 A−1 ∗ 2
 ∗ 2
Z P) − [ M(Z−1 D) + E /c + me + mp ]  M(Z P) − M(Z−1 D) − M(1 H) − E /c . (3.115)
 M(A A A−1 1

Thus, for proton decay to occur and leave the daughter in the ground state (E ∗ = 0), it is necessary that
Z P) > M(Z−1 D) − M(1 H).
A−1
M(A 1
84 Basic Atomic and Nuclear Physics Chap. 3

Internal Conversion
Often the daughter nucleus is left in an excited state, which decays (usually within about 10−9 s) to the
ground state by the emission of one or more gamma photons. However, the excitation may also be transferred
to an atomic electron (usually a K-shell electron) causing it to be ejected from the atom leaving the nucleus
in the ground state but the atom singly ionized with an inner electron-shell vacancy. Symbolically,

A ∗
IC decay: ZP −→ [A + 0
Z P] + −1 e. (3.116)

The inner electrons are very tightly bound to the nucleus with large binding energies BEeK for K-shell
electrons in heavy atoms. The amount of kinetic energy shared by the recoil ion and the ejected electron
should take this into account. The Q value for the IC decay is calculated as follows:

Z P ) − [M ([Z P] ) + me ]
QIC /c2 = M(A A +

 ∗ 2
  A 
 M(AZ P) + E /c − [ M (Z P) − me + BEK
e /c
2
+ me ]

= [E ∗ − BEK 2
e ]/c . (3.117)

This decay energy is divided between the ejected electron and the daughter ion. To conserve the zero
initial linear momentum, the daughter and IC electron must divide the decay energy as
 
M(AZ P)
Ee = [E ∗ − BEK ∗
e ]  E − BEe
K
(3.118)
M(A
Z P) + m e

and  
me
ED = A
[E ∗ − BEK
e ]  0. (3.119)
M(Z P) + me
Besides the monoenergetic IC electron, other radiation is also emitted in the IC process. As the outer
electrons cascade down in energy to fill the inner-shell vacancy, x rays and Auger electrons are also emitted.

3.7.4 Exponential Decay


Radioactive decay is a stochastic process, i.e., one cannot predict when a particular radionuclide will decay.
All that one can do is make probability statements about when it will decay. For example, as shown in this
section, one can, at best, calculate the probability that it will or will not decay in a finite time interval t.
Each radionuclide species has its own characteristic decay constant λ which is the probability a radionu-
clide decays in a unit time for an infinitesimal time interval. The smaller λ, the more slowly the radionuclides
decay. For stable nuclides, λ = 0. The decay constant for a radionuclide is independent of most experimental
parameters such as temperature and pressure, since it depends only on the nuclear forces inside the nucleus.
Consider a sample composed of a large number of identical radionuclides with decay constant λ. With
a large number of radionuclides (N >>> 1), one can use continuous mathematics to describe an inherently
discrete process. In other words, N (t) is interpreted as the average or expected number of radionuclides in
the sample at time t, a continuous quantity. Then, the probability any one radionuclide decays in an interval
dt is λdt, so the expected number of decays in the sample that occurs in dt at time t is λ dt N (t). This must
equal the decrease −dN in the number of radionuclides in the sample, i.e., −dN = λN (t)dt, or
dN (t)
= −λN (t). (3.120)
dt
Sec. 3.7. Radioactivity 85

The solution of this differential equation is

N (t) = N (0)e−λt , (3.121)

where N (0) is the number of radionuclides in the sample at t = 0. This exponential decay of a radioactive
sample is known as the radioactive decay law. Such an exponential variation with time not only applies to
radionuclides, but to any process governed by a constant rate of change, such as decay of excited electron
states of an atoms, the rate of growth of money earning compound interest, and the growth of human
populations, to name a few such processes.

3.7.5 The Half-Life


Any dynamic process governed by exponential decay has a remarkable property. The time it takes for it to
decay to one-half of the initial value, T1/2 , is a constant called the half-life. From Eq. (3.121)

No
N (T1/2 ) ≡ = No e−λT1/2 . (3.122)
2
Solving for T1/2 yields

ln 2 0.693
T1/2 =  . (3.123)
λ λ

Notice that the half-life is independent of time t. Thus, after n half-lives, the initial number of radionu-
clides has decreased by a multiplicative factor of 1/2n , i.e.,

1
N (nT1/2 ) = No . (3.124)
2n
The number of half-lives n needed for a radioactive sample to decay to a fraction  of its initial value is found
from
N (nT1/2 ) 1
≡ = n
No 2
which, upon solving for n, yields
ln 
n=−  −1.44 ln . (3.125)
ln 2
Alternatively, the radioactive decay law of Eq. (3.121) can be expressed in terms of the half-life as
 t/T1/2
1
N (t) = No . (3.126)
2

3.7.6 Decay Probability for a Finite Time Interval


From the exponential decay law, some useful probabilities and averages can be obtained. If we have No
identical radionuclides at t = 0, we expect to have No e−λt atoms at a later time t. Thus, the probability P
that any one of the atoms does not decay in a time interval t is

N (t)
P (t) = = e−λt . (3.127)
N (0)
86 Basic Atomic and Nuclear Physics Chap. 3

The probability P that a radionuclide does decay in a time interval t is

P (t) = 1 − P (t) = 1 − e−λt . (3.128)

As the time interval becomes very small, i.e., t → Δt  1, it is seen that


1
P (Δt) = 1 − e−λΔt = 1 − 1 − λΔt + (λΔt)2 − + . . .  λΔt. (3.129)
2!
This approximation is in agreement with the earlier interpretation of the decay constant λ as being the decay
probability per infinitesimal time interval.
From these results, the probability distribution function for when a radionuclide decays can be obtained.
Specifically, let p(t)dt be the probability a radionuclide, which exists at time t = 0, decays in the time interval
between t and t + dt. Clearly,

p(t)dt = {prob. it doesn’t decay in (0, t)} {prob. it decays in the next dt time interval}
   
= P (t) {P (dt)} = e−λt {λ dt} = λe−λt dt. (3.130)

3.7.7 Mean Lifetime


In a radioactive sample, radionuclides decay at all times. From Eq. (3.121) it is seen that an infinite time
is required for all the radioactive atoms to decay. However, as time increases, fewer and fewer atoms decay.
The average lifetime of a radionuclide can be obtained by using the decay probability distribution p(t)dt of
Eq. (3.130). The average or mean lifetime Tav of a radionuclide is thus
 ∞  ∞ ∞  ∞
−λt

−λt  1
Tav = t p(t) dt = tλe dt = −te  + e−λt dt = . (3.131)
0 0 0 0 λ

40
Example 3.3: What is the value of the decay constant and the mean lifetime of K (half-life 1.29 Gy)?

Solution:
The decay constant is
ln 2 ln 2
λ= = = 5.37 × 10−10 y−1 .
T1/2 1.29 × 109 y
The average lifetime is t = 1/λ = 1.86 × 109 y.

3.7.8 Activity
For detection and safety purposes, one is generally not really interested in the number of radioactive atoms
in a sample; rather one is interested in the number of decays or transmutations per unit of time that occur
within the sample. This decay rate, or activity A(t), of a sample is given by17
dN (t)
A(t) ≡ − = λN (t) = λNo e−λt = Ao e−λt , (3.132)
dt
where Ao is the activity at t = 0. Since the number of radionuclides in a sample decreases exponentially, the
activity also decreases exponentially.

17 Do not confuse the symbol A used here for activity with the same symbol used for the atomic mass number.
Sec. 3.7. Radioactivity 87

The SI unit used for activity is the becquerel (Bq) and is defined as one transformation per second. An
older unit of activity, and one that is still sometimes encountered, is the curie (Ci) defined as 3.7 × 1010 Bq.
One Ci is the approximate activity of one gram of 226 88 Ra (radium). To obtain 1 Ci of tritium (T1/2 = 12.6 y,
λ = 1.74 × 10−9 s−1 ) one needs 1.06×10−4 g of tritium. By contrast, one Ci of 238 U (λ = 4.88 × 10−18 s−1 )
is 3.00×106 g.

3.7.9 Decay by Competing Processes


Some radionuclides decay by more than one process. For example, 64 29 Cu
*

64
30 Zn (β − 39.0%)
 decays by β + emission 17.4% of the time, by β − emission 39.0% of the
64   - 64 +
29 Cu HH 28 Ni (β 17.4%) time, and by electron capture 43.6% of the time, as shown in Fig. 3.24.
Hj
H 64 Each decay mode is characterized by its own decay constant λi . For the
28 Ni (EC 43.6%)
present example of 64
29 Cu, the decay constants for the three decay modes
62
Figure 3.24. 29 Cu has three ra- are λβ + = 0.009497 h−1 , λβ − = 0.02129 h−1 , and λEC = 0.02380 h−1 .
dioactive decay modes. To find the effective decay constant when the decay process has n
competing decay modes, write the differential equation that models the rate of decay. Denote the decay
constant for the ith mode by λi . Thus, the rate of decay of the parent radionuclide is given by,

dN (t) n
= −λ1 N (t) − λ2 N (t) − · · · − λn N (t) = − λi N (t) ≡ −λN (t). (3.133)
dt i=1

where λ is the overall decay constant, namely,


n
λ≡ λi . (3.134)
i=1

The probability fi that the nuclide will decay by the ith mode is

decay rate by ith mode λi


fi = = . (3.135)
decay rate by all modes λ

3.7.10 Decay Dynamics


The transient behavior of the number of atoms of a particular radionuclide in a sample depends on the
nuclide’s rates of production and decay, the initial values of it and its parents, and the rate at which it
escapes from the sample. In this section, several common decay transients are discussed.

Decay with Production


In many cases the decay of radionuclides is accompanied by the creation of new ones, either from the decay
of a parent or from production by nuclear reactions such as cosmic ray interactions in the atmosphere or
from neutron interactions in a nuclear reactor. If Q(t) is the rate at which the radionuclide of interest is
being created, the rate of change of the number of radionuclides is

dN (t)
= −rate of decay + rate of production (3.136)
dt
or
dN (t)
= −λN (t) + Q(t). (3.137)
dt
88 Basic Atomic and Nuclear Physics Chap. 3

The most general solution of this differential equation is

 t

N (t) = No e−λt + dt Q(t )e−λ(t−t ) (3.138)
0

where again No is the number of radionuclides at t = 0.


For the special case that Q(t) = Qo (a constant production rate), the integral in Eq. (3.138) can be
evaluated analytically to give
Qo
N (t) = No e−λt + [1 − e−λt ]. (3.139)
λ
As t → ∞ it is seen that N (t) → Ne = Qo /λ, where Ne is the equilibrium value. This constant equilibrium
value Ne can be obtained more directly from Eq. (3.137). Upon setting the left-hand side of Eq. (3.137) to
zero (the equilibrium condition), it is seen that 0 = −λNe + Qo , or Ne = Qo /λ.

Three Component Decay Chains


Often a radionuclide decays to another radionuclide which in turn decays to yet another. The chain continues
until a stable nuclide is reached. For simplicity, first consider a three-component chain. Such three component
chains are quite common and an example is

T1/2 =29.1y 90 T1/2 =64h


90
38 Sr −→ 39 Y −→ 90 40 Zn( stable),

in which both radionuclides decay by β − emission. Such three-member decay chains can be written schemat-
ically as
1λ 2 λ
X1 −→ X2 −→ X3 ( stable).

At t = 0 the number of atoms of each type in the sample under consideration is denoted by Ni (0), i =
1, 2, 3. The differential decay equations for each species are (assuming no loss from or production in the
sample)

dN1 (t)
= −λ1 N1 (t). (3.140)
dt
dN2 (t)
= −λ2 N2 (t) + λ1 N1 (t). (3.141)
dt
dN3 (t)
= λ2 N2 (t). (3.142)
dt
The solution of Eq. (3.140) is just the exponential decay law of Eq. (3.121), i.e.,

N1 (t) = N1 (0)e−λ1 t . (3.143)

The number of first daughter atoms N2 (t) is obtained from Eq. (3.138) with the production term Q(t) =
λ1 N1 (t). The result is
λ1 N1 (0) −λ1 t
N2 (t) = N2 (0)e−λ2 t + [e − e−λ2 t ]. (3.144)
λ2 − λ1
Sec. 3.7. Radioactivity 89

The number of second daughter (granddaughter) atoms is obtained by integrating Eq. (3.142). Thus,
 t
N3 (t) = N3 (0) + λ2 dt N2 (t )
0
 t  t
 N1 (0)λ1 λ2  
= N3 (0) + λ2 N2 (0) dt e−λ2 t + dt [e−λ1 t −e−λ2 t ]
0 λ2 − λ1 0

N1 (0)
= N3 (0) + N2 (0)[1−e−λ2 t ] + [λ2 (1−e−λ1 t )−λ1 (1−e−λ2 t )]. (3.145)
λ2 − λ1
General Decay Chain
The general decay chain can be visualized as
λ
1 2 3 λ λ λ λn−1
X1 −→ X2 −→ X3 −→ · · · Xi −→
i
· · · −→ Xn (stable)

The decay and buildup equations for each member of the decay chain are

dN1 (t)
= −λ1 N1 (t)
dt
dN2 (t)
= λ1 N1 (t) − λ2 N2 (t)
dt
dN3 (t)
= λ2 N2 (t) − λ3 N3 (t)
dt
.. ..
. .
dNn−1 (t)
= λn−2 Nn−2 (t) − λn−1 Nn−1 (t)
dt
dNn (t)
= λn−1 Nn−1 (t). (3.146)
dt
For the case when only radionuclides of the parent X1 are initially present, the initial conditions are
N1 (0) = 0 and Ni (0) = 0, i > 1. The solution of these so-called Bateman equations with these initial
conditions is [Faw and Shultis 1999]


j
Aj (t) = λj Nj (t) = N1 (0)(C1 e−λ1 t + C2 e−λ2 t + · · · + Cj e−λj t ) = N1 (0) Cm e−λm t . (3.147)
m=1

The coefficients Cm are


j
i=1 λi λ1 λ2 λ3 · · · λj
Cm = j = , (3.148)
− λm ) (λ1 − λm )(λ2 − λm ) · · · (λj − λm )
i=1 (λi
i=m

where the i = m term is excluded from the denominator.


90 Basic Atomic and Nuclear Physics Chap. 3

PROBLEMS

1. In 1911, Robert A. Millikan determined the singular charge held by an electron. In the experiment,
parallel metal plates were fashioned as depicted in Fig. 1.14 with a voltage applied. Millikan would
discharge an atomized cloud of oil droplets into the chamber. Free electrons would attach to oil droplets,
and an appropriate adjustment of the voltage would allow the electric force on the oil droplet to equal
the gravitational force, thereby suspending such an oil droplet motionless in the chamber. Calculate
the change in voltage needed to suspend an oil droplet onto which three electrons have attached. The
electron charge is 1.602 × 10−19 C.

2. For slowly moving particles, that is, v  c, show that Eq. (3.8) yields the usual classical result,

1
T = mc2 − mo c2  mo v 2 . (3.149)
2

3. An accelerator increases the kinetic energy of electrons uniformly to 10 GeV over a 3000 m path. That
means that at 30 m, 300 m, and 3000 m, the kinetic energy is 108 , 109 , and 1010 eV, respectively. At
each of these distances, compute the velocity, relative to light (v/c), and the mass in atomic mass units.

4. Muons are subatomic particles that have the negative charge of an electron but are 206.77 times more
massive. They are produced high in the atmosphere by cosmic rays colliding with nuclei of oxygen or
nitrogen, and muons are the dominant cosmic-ray contribution to background radiation at the earth’s
surface. A muon, however, rapidly decays into an energetic electron, existing, from its point of view,
for only 2.20 μs, on the average. Cosmic-ray generated muons typically have speeds of about 0.998c
and thus should travel only a few hundred meters in air before decaying. Yet muons travel through
several kilometers of air to reach the earth’s surface. Using the results of special relativity, explain how
this is possible. HINT: consider the atmospheric travel distance as it appears to a muon, and the muon
lifetime as it appears to an observer on the earth’s surface.

5. A 1-MeV gamma ray loses 200 keV in a Compton scatter. Calculate the scattering angle.

6. At what energy (in MeV) can a photon lose at most one-half of its energy in Compton scattering?

7. What is the de Broglie wavelength of a water molecule moving at a speed of 2400 m/s? What is the
wavelength of a 3-g bullet moving at 400 m/s?

8. If a neutron is confined somewhere inside a nucleus of characteristic dimension Δx  10−14 m, what


is the uncertainty in its momentum Δp? For a neutron with momentum equal to Δp, what is its total
energy and its kinetic energy in MeV? Verify that classical expressions for momentum and kinetic energy
may be used.

9. Repeat the previous problem for an electron trapped in the nucleus. HINT: relativistic expressions for
momentum and kinetic energy must be used.

10. Estimate the wavelengths of the first three spectral lines in the Lyman spectral series for hydrogen.
What energies (eV) do photons with these wavelengths have?

11. Consider an electron in the first Bohr orbit of a hydrogen atom. (a) What is the radius (in meters) of
this orbit? (b) What is the total energy (in eV) of the electron in this orbit? (c) How much energy is
required to ionize a hydrogen atom when the electron is in the ground state?
Problems 91

12. What photon energy (eV) is required to excite the hydrogen electron in the innermost (ground state)
Bohr orbit to the first excited orbit?

13. What is the de Broglie wavelength of the electron in the first Bohr orbit? Compare this wavelength to
the circumference of the first Bohr orbit. What does this comparison reveal about the standing wave in
the first Bohr orbit?

14. Calculate the limiting (smallest) wavelength of the Lyman, Balmer, and Paschen series for the Bohr
model of the hydrogen atom.

15. What is the net energy released (in MeV) for each of the following fusion reactions? (a) 21 H + 21 H −→
2 He + 0 n and (b) 1 H + 1 H −→ 2 He + 0 n.
3 1 2 3 4 1

Data: M (21 H) = 2.0141018 u; M (31 H) = 3.0160493 u;


M (32 He) = 3.0160293 u; M (42 He) = 4.0026032 u; mn = 1.0086649 u, .

16. Calculate the Q-values for the following two beta radioactive decays.
11 Na −→ 10 Ne + +1 e + ν and (b) M 17 Cl −→ 18 Ar + −1 e + ν.
(a) 22 22 0 38 38 0

Data: M (22 22
11 Na) = 21.9944368 u; M (10 Ne) = 21.9913855 u;
M (17 Cl) = 37.9680106 u; M (18 Ar) = 37.9637322 u; me = 5.485799 × 10−4 u. .
38 38

17. The radioisotope 224 Ra decays by α emission primarily to the ground state of 220 Rn (94% probability)
and to the first excited state 0.241 MeV above the ground state (5.5% probability). What are the
energies of the two associated α particles?
Data: M (224 220
88 Ra) = 224.0202020 u; M ( 86 Rn) = 220.0113841 u;
4
M (2 He) = 4.0026032 u;

18. The activity of a radioisotope is found to decrease by 30% in one week. What are the values of its (a)
decay constant, (b) half-life, and (c) mean life?
24 238
19. How many atoms are there in a 1.20 MBq source of (a) Na and (b) U?

20. The isotope 132 I decays by β − emission to 132 Xe with a half-life of 2.3 h. (a) How long will it take for
7/8 of the original number of 132 I nuclides to decay? (b) How long will it take for a sample of 132 I to
lose 95% of its activity?
32
21. How many grams of P are there in a 5 mCi source?

22. The average mass of potassium in the human body is about 140 g. From the abundance and half-life of
40
K (see Table 5.1), estimate the average activity (Bq) of 40 K in the body.

23. A 6.2 mg sample of 90 Sr (half-life 29.12 y) is in secular equilibrium with its daughter 90 Y (half-life
64.0 h). (a) How many Bq of 90 Sr are present? (b) How many Bq of 90 Y are present? (c) What is the
mass of 90 Y present? (d) What will the activity of 90 Y be after 100 y?

24. Consider a sample in which A is a radioactive parent that decays to a radioactive daughter B. If the
initial activity of B at t = 0 is zero, show that the maximum activity of B is reached at time
 
λB
ln
λA
tmax = A0 . (3.150)
λB − λA
92 Basic Atomic and Nuclear Physics Chap. 3

25. Using a chart of nuclides, start with 241 Am and list the daughter products and methods of decay for
each daughter product to the end of the chain (stable isotope).

REFERENCES
ESTERMANN, I., AND O. STERN, “Beugung von Moleku- POVH, B., K. RITH, C. SCHOLZ, AND F. ZETSCHE, Particles and
larstrahlen,” Z. Physik., 61, 95–125, (1930). Nuclei, 5th Ed., Berlin: Springer, 2006.
EVANS, R.D., The Atomic Nucleus, New York: McGraw-Hill, RILEY, K.F., M.P. HOBSON, AND S.J. BENCE, Mathematical Meth-
1955; republished by Melborne, FL: Krieger Publishing Co., ods for Physics and Engineering, 3rd Ed., Cambridge: Cam-
1982. bridge University Press, 2006.
FAW, R.E. AND J.K. SHULTIS, Radiological Assessment, La
SCHIFF, L.I., Quantum Mechanics, 3rd Ed., New York: McGraw
Grange Park, IL: American Nuclear Society, 1999.
Hill, 1968.
FIRESTONE, R.B., AND V.S. SHIRLEY, Eds., Table of Isotopes,
Vols. 1 and 2, 8th Ed, New York: Wiley, 1996. SHULTIS, J.K. AND R.E. FAW, Fundamentals of Nuclear Science
and Engineering, 3rd Ed., Boca Raton, FL: CRC Press, 2017.
GRIFFITHS, D.J., Introduction to Elementary Particles, Strauss:
Wiley-VCH, 2004. THOMSON, G.P., “Experiments on the Diffraction of Cathode
Rays,” Proc. Roy. Soc., 117, 600, (1928).
GRIFFITHS, D.J., Introduction of Quantum Mechanics, 2nd Ed.,
Upper Saddle River, NJ: Pearson Prentice Hall, 2005. WEBER, D.A., K.F. ECKERMAN, L.T. DILLMAN, AND J.C. RYMAN,
ICRP, Radionuclide Transformations, Publication 38, Interna- MIRD: Radionuclide Data and Decay Schemes, New York: So-
tional Commission on Radiological Protection, Annals of the ciety of Nuclear Medicine, 1989.
ICRP, 11-13, 1983. YAO, Y-M, et al., “Review of Particle Physics,” J. Phys. G., 33,
KAPLAN, I., Nuclear Physics, Reading: Addison-Wesley, 1962. 1–1232, (2006).
Chapter 4

Radiation Interactions
in Matter

Every great discovery I ever made, I gambled that the truth was there,
and then I acted in faith until I could prove its existence.
Arthur H. Compton

4.1 Introduction
It is important that any professional working with or designing radiation detectors and instrumentation be
familiar with fundamental interactions of radiation with matter. It is through these interactions that observ-
able phenomena can be manipulated to yield information about the radiation type, intensity, and energy,
as well as other possible uses, such as expected results and characteristic signatures. For radiation to be
detected, it must first interact with neutral atoms in the detector and produce ionization and/or excitation in
the detector material. Ionizing radiation is generally subdivided into two classes: directly ionizing radiation
whose interactions produce ionization and excitation in a medium, and indirectly ionizing radiation that
cannot ionize atoms but that can cause interactions whose charged products, known as secondary radiation,
are directly ionizing. Fast moving charged particles, such as alpha particles, beta particles and fission frag-
ments, can directly ionize and excite matter. Neutral particles, such as neutron and photons, cannot interact
Coulombically with the electrons of the matter through which they pass; rather they cause interactions that
transfer some of their incident kinetic energy to charged secondary particles.
In this chapter, how these two types of ionizing radiation interact with matter is discussed. Particular
emphasis is given to quantifying the rate at which the radiation interacts with the medium and how the
kinetic energy of the radiation is transfered to the medium.

4.2 Indirectly Ionizing Radiation


First considered is indirectly ionizing radiation whose particles carry no charge. Of primary concern are
the interactions of photons and neutrons, although the general principles discussed here also apply to other
neutral particles such as neutrinos and neutral mesons. Later in the chapter the interaction of directly
ionizing radiation is considered.

4.2.1 Attenuation of Neutral Particle Beams


The interaction of a photon or neutrons with constituents of matter is dominated by short-range forces.
Consequently, unlike charged particles, neutral particles move in straight lines through a medium, punctuated
by occasional “point” interactions, in which the neutral particle may be absorbed or scattered or cause some

93
94 Radiation Interactions in Matter Chap. 4

other type of reaction. The interactions are stochastic in nature, i.e., the travel distance between interactions
with the medium can be predicted only in some average or expected sense.
The interaction of a given type of neutral radiation with matter may be classified according to the type
of interaction and the matter with which the interaction takes place. The interaction may take place with
an electron, and in many cases the electron behaves as though it were free. Similarly, the interaction may
take place with an atomic nucleus, which in many cases behaves as though it were not bound in a molecule
or crystal lattice. However, in some cases, particularly for radiation particles of comparatively low energy,
molecular or lattice binding must be taken into account.
The interaction may be a scattering of the incident radiation accompanied by a change in its energy. A
scattering interaction may be elastic or inelastic. Consider, for example, the interaction of a gamma photon
with an electron in what is called Compton scattering. In the sense that the interaction is with the entire
atom within which the electron is bound, the interaction must be considered as inelastic, since some of the
incident photon’s energy must compensate for the binding energy of the electron in the atom. However, in
most practical cases, electron binding energies are orders of magnitude lower than gamma-photon energies,
and the interaction may be treated as a purely elastic scattering of the photon by a free electron. Neutron
scattering by an atomic nucleus may be elastic, in which case the incident neutron’s kinetic energy is shared
by that of the scattered neutron and that of the recoil nucleus, or it may be inelastic, in which case, some of
the incident neutron’s kinetic energy is transformed to internal energy of the nucleus and thence to a gamma
ray emitted from the excited nucleus. It is important to note that, for both elastic and inelastic scattering,
unique relationships between energy exchanges and angles of scattering arise from conservation of energy
and linear momentum.
Other types of interactions are absorptive in nature. The identity of the incident particle is lost, and
total relativistic momentum and energy are conserved, some of the energy appearing as nuclear excitation
energy, some as translational, vibrational, and rotational energy. The ultimate result may be the emission
of particulate radiation, as occurs in the photoelectric effect and in neutron radiative capture.
The discussion in this section of how a beam of radiation is attenuated as it passes through matter
applies equally to both neutrons and photons. In later sections, descriptions specific to each type of neutral
radiation and the particular radiation-medium interactions involved are given. The concept of the interaction
coefficient is first introduced to describe how readily radiation particles interact with matter, and then use
it to quantify the attenuation of a beam of neutral particles passing through some material.

4.2.2 The Linear Interaction Coefficient


The interaction of radiation with matter is always statistical in nature, and, therefore, must be described
in probabilistic terms. Consider a particle traversing a homogeneous material and let Pi (Δx) denote the
probability that this particle, while traveling a distance Δx in the material, causes a reaction of type i (e.g., it
is scattered). It is found empirically that the probability per unit distance traveled, Pi (Δx)/Δx, approaches
a constant as Δx becomes very small, i.e.,
Pi (Δx)
μi ≡ lim . (4.1)
Δx→0 Δx
The quantity μi is a property of the material for a given incident particle and interaction. In the limit of
small path lengths, μi is seen to be the probability, per unit differential path length of travel, that a particle
undergoes an ith type of interaction.
That μi is constant for a given material and for a given type of interaction implies that the probability
of interaction, per unit differential path length, is independent of the path length traveled prior to the
interaction. In this book, when the interaction coefficient is referred to as the probability per unit path length
of an interaction, it is understood that this is true only in the limit of very small path lengths.
Sec. 4.2. Indirectly Ionizing Radiation 95

The constant μi is called the linear coefficient for reaction i. For each type of reaction, there is a
corresponding linear coefficient. For, example, μa is the linear absorption coefficient, μs the linear scattering
coefficient, and so on. Although this nomenclature is widely used to describe photon interactions, μi is often
referred to as the macroscopic cross section for reactions of type i, and is usually given the symbol Σi when
describing neutron interactions. In this section, the photon jargon is used, although the present discussion
applies equally to neutrons.
The probability, per unit path length, that a neutral particle undergoes some sort of reaction, μt , is the
sum of the probabilities, per unit path length of travel, for each type of possible reaction, i.e.,

μt (E) = μi (E). (4.2)
i

Because these coefficients generally depend on the particle’s kinetic energy E, this dependence has been
shown explicitly. The total interaction probability per unit path length, μt , is fundamental in describing
how indirectly ionizing radiation interacts with matter and is usually called the linear attenuation coefficient.
It is perhaps more appropriate to use the words total linear interaction coefficient since many interactions
do not “attenuate” the particle in the sense of an absorption interaction.

4.2.3 Attenuation of Uncollided Radiation


- Consider a plane parallel beam of neutral particles of intensity Io par-
- ticles cm−2 s−1 normally incident on the surface of a thick slab (see
- -
- - Fig. 4.1). As the particles pass into the slab, some interact with the
I o (x) -
- - slab material. Of interest in many situations, is the intensity I o (x) of
- uncollided particles at depth x into the slab. At some distance x into
- - o
I (x + dx)
I o (0) - the slab, some uncollided particles undergo interactions for the first
- -
- time as they cross the next Δx of distance, thereby reducing the uncol-
- - lided beam intensity at x, I o (x), to some smaller value I o (x + Δx) at
- - x + Δx. The probability an uncollided particle interacts as it crosses
-
- - Δx is
- - I o (x) − I o (x + Δx)
P (Δx) = .
I o (x)
0 x x + dx
distance into slab In the limit as Δx → 0, Eq. (4.1) yields
Figure 4.1. Uniform illumination
P (Δx) I o (x) − I o (x + Δx) 1 dI o (x) 1
of a slab by radiation. μt = lim = lim ≡ −
Δx→0 Δx Δx→0 Δx I o (x) dx I o (x)
or
dI o (x)
= −μt I o (x). (4.3)
dx
The solution for the uncollided intensity is

I o (x) = I o (0)e−μt x . (4.4)

Uncollided, indirectly ionizing radiation is thus exponentially attenuated as it passes through a medium.
From this result, the interaction probability P (x) that a particle interacts somewhere along a path of
length x is
I o (x)
P (x) = 1 − o = 1 − e−μt x . (4.5)
I (0)
96 Radiation Interactions in Matter Chap. 4

The probability P (x) that a particle does not interact while traveling a distance x is

P (x) = 1 − P (x) = e−μt x . (4.6)

As x → dx, it is found that P (dx) → μt dx, which is in agreement with the definition of μt .

4.2.4 Average Travel Distance Before an Interaction


From the above results, the probability distribution for how far a neutral particle travels before interacting
can be derived. Let p(x)dx be the probability that a particle interacts for the first time between x and
x + dx. Then

p(x)dx = {prob. particle travels a distance x without interaction} × {prob. it interacts in the next dx}
   
= P (x) {P (dx)} = e−μt x {μt dx} = μt e−μt x dx. (4.7)
∞
Note that 0 p(x) dx = 1, as is required for a proper probability distribution function.
This probability distribution can be used to find the average distance x traveled by a neutral particle to
the site of its first interaction, namely, the average distance such a particle travels before it interacts. The
average of x is  ∞  ∞
1
x= x p(x) dx = μt x e−μt x dx = . (4.8)
0 0 μt

This average travel distance before an interaction, 1/μt , is called the mean-free-path length.
The total linear attenuation coefficient μt can be interpreted, equivalently, as (1) the probability, per unit
differential path length of travel, that a particle interacts, or (2) the inverse of the average distance traveled
before interacting with the medium. Note the analogy to radioactive decay, where the decay constant λ is
the inverse of the mean lifetime of a radionuclide.

4.2.5 Half-Thickness
To estimate how incident radiation interacts in a detector medium, a convenient concept is that of the half-
thickness, x1/2 , namely, the thickness of a medium required for half of the incident radiation to undergo an
interaction. For the uncollided beam intensity to be reduced to one-half of its initial value, x1/2 must be
such that
1 I o (x1/2 )
= = e−μt x1/2
2 I o (0)
from which one finds
ln 2
x1/2 = . (4.9)
μt
Again, note the similarity to the half-life of radioactive decay.

4.2.6 Microscopic Cross Sections


The linear coefficient μi (E) depends on the type and energy E of the incident particle, the type of interaction
i, and the composition and density of the interacting medium. One of the more important quantities that
determines μ is the density of target atoms or electrons in the material. It seems reasonable to expect that
μi should be proportional to the “target” atom density N in the material, that is,

ρN
μi = σi N = σi A a , (4.10)
Sec. 4.2. Indirectly Ionizing Radiation 97

where σi is a constant of proportionality independent of N . Here ρ is the mass density of the medium, Na
is Avogadro’s number (mol−1 ), and A is the atomic weight of the medium.
The proportionality constant σi is called the microscopic cross section for reaction i, and is seen to
have dimensions of area. It is often interpreted as being the effective cross-sectional area presented by
the target atom to the incident particle for a given interaction. Indeed, in many cases σi has dimensions
comparable to those expected from the physical size of the nucleus. However, this simplistic interpretation
of the microscopic cross section, although conceptually easy to grasp, leads to philosophical difficulties when
it is observed that σi generally varies with the energy of the incident particle and, for a crystalline material,
the particle direction. The view that σ is the interaction probability per unit differential path length,
normalized to one target atom per unit volume, avoids such conceptual difficulties while emphasizing the
statistical nature of the interaction process. Cross sections are usually expressed in units of cm2 . A widely
used special unit is the barn, equal to 10−24 cm2 .
Data on cross sections and linear interaction coefficients, especially for photons, are frequently expressed
as the ratio of μi to the density ρ, called the mass interaction coefficient for reaction i. Upon division of
Eq. (4.10) by ρ, one obtains
μi σi N Na
= = σi . (4.11)
ρ ρ A
From this result, it is seen that μi /ρ is an intrinsic property of the interacting medium—independent of its
density. This method of data presentation is used much more for photons than for neutrons, in part because,
for a wide variety of materials and a wide range of photon energies, μi /ρ is only weakly dependent on the
nature of the interacting medium.
For compounds or homogeneous mixtures, the linear and mass interaction coefficients for interactions of
type i are, respectively,
 j 
μi = μi = N j σij (4.12)
j j

and
 j
μi  μi
= wj , (4.13)
ρ j
ρ

in which the superscript j refers to the jth component of the material, the subscript i to the type of
interaction, and wj is the weight fraction of component j. In Eq. (4.12), the atomic density N j and the
linear interaction coefficient μji are values for the jth material after mixing.

4.2.7 Calculation of Radiation Interaction Rates


To quantify the number of interactions caused by neutral particles as they pass through matter, one often
needs to estimate the number of a specific type of interaction that occurs, in a unit time and in a unit
volume, at some point in the matter. This density of reactions per unit time is called the reaction rate
density, denoted by Fi . This quantity depends on (1) the amount or strength of the radiation at the point
of interest, and (2) the readiness with which the radiation can cause the interaction of interest.

Flux Density
At any given location r, the radiation field is generally a function of time t (e.g., a detector can pass by
a radiation source) and of the radiation particles’ energy E (e.g., radiation sources often emit photons or
neutrons with many energies). To quantify the “strength” of a radiation field one could use the particle
density n(r, E, t) where n(r, E, t)dV dE is the expected number of particles in differential volume element
98 Radiation Interactions in Matter Chap. 4

dV about r with energies in dE about E at time t. Alternatively, one could use the flux density, often just
called the flux, which is defined as
φ(r, E, t) ≡ v(E) n(r, E, t), (4.14)
where v(E) is the speed of a radiation particle with kinetic energy E.1
Because v(E) is the distance a radiation particle of energy E travels in a unit time, the flux φ(r, E, t)dV dE
has the interpretation of being the distance traveled in a unit time by particles in dV and r that have energies
in dE and E.
Reaction-Rate Density
With the concepts of flux and interaction coefficient, the rate at which radiation interacts with a medium
can be quantified. Specifically, let Fi (r, E, t)dE be the expected number of ith type interactions per unit
time that occurs in a unit volume at r caused by radiation particles with energies in dE about E. Thus,

Fi (r) = {total path-length traveled by the particles in one cm3 in one second}/
{average distance particles must travel for an ith type interaction

= {φ(r, E, t)dE}/{1/μi (r, E, t)}

or

Fi (r, E, t)dE = μi (r, E, t) φ(r, E, t)dE. (4.15)

This simple expression for reaction-rate densities is a key equation for many nuclear calculations.
From the interaction rate density, all sorts of useful information can be calculated about the effects of
the radiation. For example, the total number of scattering interactions that occur in some detector volume
V between times t1 and t2 by radiation particle of all energies is
 t2   Emax
Number of scatters in (t1 , t2 ) = dt dV dE μs (r, E, t)φ(r, E, t). (4.16)
t1 V 0

Finally, to obtain the reaction rate density per unit mass, simply replace μ in the above expression by (μ/ρ),
where ρ is the mass density of the interacting medium.
Radiation Fluence
In most interaction rate calculations, the interaction properties of the medium do not change appreciably in
time. For this usual situation, the example of Eq. (4.16) reduces to
  Emax
Number of fissions in (t1 , t2 ) = dV dE Σf (r, E) Φ(r, E), (4.17)
V 0

where the fluence of radiation between t1 and t2 is the time-integrated flux density, namely

 t2
Φ(r, E) ≡ dt φ(r, E, t). (4.18)
t1

1 Photons, of course, always travel with the speed of light so v(E) = c. However, neutrons of different energies have different
speeds.
Sec. 4.3. Scattering Interactions 99

For a steady-state radiation field, the fluence is simply Φ(r, E) = (t2 − t1 )φ(r, E).
Often the time interval over which the flux density is integrated to obtain the fluence is implicitly assumed
to be over all prior time. Thus, the fluence at time t is
 t
Φ(r, E, t) ≡ dt φ(r, E, t ). (4.19)
−∞

The rate of change of the fluence with time, or the fluence rate, is simply the flux density. The fluence is thus
used to quantify the cumulative effect of radiation interactions, while the flux density is used to quantify the
rate of interactions.

4.3 Scattering Interactions


Scattered radiation is of great concern in interpreting the results of radiation detectors. First scattering
transfers a spectrum of energies to the scattering medium as a result of the many different scattering angles
that can occur. Likewise scattering of radiation from material near a detector cause radiation with a great
variety of energies to reach a detector.

4.3.1 Differential Scattering Coefficients


The scattering coefficient μs is generally a function of the energy of the incident radiation. However, to
describe the many features of a scattering interaction, μs may depend on other variables, leading to so-called
differential scattering coefficients. Such coefficients may be a function of (1) the energy of the particle after
scattering, (2) the energy of the recoil atom or electron, (3) the angles of deflection of the scattered radiation
and recoil atom or electron,2 and (4) the angles of emission of secondary particles.
For example, the doubly differential scattering interaction coefficient is defined in such a way that
d2 μs (E, E  , θs )/dE  dΩs is the probability per unit path length for an interaction in which the incident parti-
cle of energy E emerges from the interaction with energy between E  and E  + dE  and with scattering angle
θs , measured with respect to the incident direction, within the differential solid angle dΩs .3 In this form, μ
has units such as cm−1 MeV−1 sr−1 . Alternatively, the interaction coefficient could be expressed in terms of
energy Tr and angles θr for recoil electrons or atoms, or other secondary radiations. Thus, one has an equiva-
lent doubly differential scattering interaction coefficient d2 μs (E, Tr , θr )/dTr dΩr = d2 μs (E, E  , θs )/dE  dΩs .
This later description is most useful for radiation detection, because it is the energy of recoil secondary
radiation that is of interest, i.e., the energy deposited in the detector.
Often it is also of interest to deal only with, say, the energy dependence or the angular distribution of
scattered radiation. In this case, one or the other of the following forms of singly differential scattering
coefficient may be used:

dμs (E, Tr ) d2 μs (E, Tr , θr )
≡ dΩr (4.20)
dTr 4π dTr dΩr
or  ∞
dμs (E, θr ) d2 μs (E, Tr , θr )
≡ dTr . (4.21)
dΩr 0 dTr dΩr
Here dμs (E, Tr )/dTr is the probability, per unit path length of travel, that scattering produces a recoil particle
with energy dTr about Tr , without regard to scattering angle. Likewise, dμs (E, θr )/ dΩr is the probability

2 This dependence is true for isotropic media, which is assumed to be the case unless otherwise noted specifically. For crystalline
and other anisotropic media, μs generally depends on the incident radiation direction Ω and the exit radiation direction Ω .
3 In many references the differential coefficient d2 μ (E, E  , θ )/dE  dΩ is simply written as μ (E, E  , θ ).
s s s s s
100 Radiation Interactions in Matter Chap. 4

for scattering into direction range dΩr , without regard to the energy of the exit radiation. Finally,
 ∞ 
dμs (E, Tr ) dμs (E, θr )
μs (E) ≡ dTr ≡ dΩr , (4.22)
0 dT r 4π dΩr
which is just the total linear interaction coefficient for the scattering of incident radiation of energy E,
without regard to the recoil particle’s energy or angle of recoil. Associated with the differential scattering
coefficients are the differential microscopic scattering cross sections as a generalization of Eq. (4.10). For
example
d2 μs (E, E  , θs ) d2 σs (E, E  , θs ) ρNa d2 σs (E, E  , θs )
= N = . (4.23)
dE  dΩs dE  dΩs A dE  dΩs

4.3.2 Conservation Laws for Scattering Reactions


Conservation of Momentum
Consider the nuclear reaction illustrated in Fig. 4.2. Reactants are a stationary target of rest mass M and
an incident particle of rest mass m, kinetic energy E, and momentum p. Products are one particle of rest
mass m , kinetic energy E  , and momentum p , and a second particle of rest mass M  , kinetic energy T , and
momentum pr . Energies E, E  , and T are kinetic energies in the laboratory system, except for photons for
which the adjective kinetic is not used.

E’
p
r
p’
qs qs
qr
E
p
qr

T
(a) (b)

Figure 4.2. Nuclear reaction with one reactant initially stationary and
with products emerging at angles θs and θr in the laboratory system. (a)
Energies and scattering angles. (b) Conservation of linear momentum.

Energy and momentum of the incident particle are related by the equation

E = p2 c2 + m2 c4 − mc2 , (4.24)

in which scalar p is the magnitude of the momentum p and c is the speed of light in vacuum, 2.9979 × 108
m/s. Similar equations relate E  and p , and T and pr . Conservation of linear momentum is depicted in
the vector diagram Fig. 4.2(b), in which the initial momentum vector p must equal the sum of the product
momentum vectors p and pr . From the law of cosines,

(p )2 = p2 + p2r − 2ppr cos θr (4.25)

and
p2r = p2 + (p )2 − 2pp cos θs . (4.26)
Sec. 4.3. Scattering Interactions 101

It is also clear from the figure that from the law of sines,

p / sin θr = pr / sin θs . (4.27)

Conservation of Energy
The fact that total energy, the sum of kinetic and rest-mass energy, is conserved in the nuclear reaction is
expressed by the equation
E = E  + T − Q, (4.28)
in which Q is the Q value of the reaction. If it is assumed that the reactants are initially in the ground state,
i.e., m = mo and M = Mo , the Q value is given by

Q = ΔMo c2 − W ≡ (mo + Mo − mo − Mo )c2 − Eex , (4.29)

in which ΔMo c2 is energy equivalent of the changes in the ground-state rest masses of the reactants, and W
is the sum of the nuclear excitation energies Eex of the reaction products.
Application of the Conservation Laws
If an incident particle is a photon, the rest mass is zero and, from Eq. (4.24), p = E/c. If the incident
particle is√a neutron, classical mechanics may be assumed to apply for energies less than about 15 MeV,
and p = 2mE. If the incident particle is an electron, then relativistic conservation laws generally should
be applied and the following equations are useful. The ratio of the particle speed to the speed of light in
vacuum is identified as β = v/c, and, with  ≡ E/mc2 , then obtains the results

( + 2) β2
β2 = , = ( + 2) (4.30)
( + 1)2 1 − β2

and
β 2 m 2 c4
p2 c2 = E(E + 2mc2 ) = . (4.31)
1 − β2
Equations (4.24) through (4.31) provide the framework for treatment of the kinematics of a large class of
nuclear reactions. They are drawn upon throughout this book. The topics now to be addressed are scattering
reactions, for which m = m and M  = M . Most reactions addressed are elastic scattering, for which the
Q value is zero. The exception is inelastic scattering of a neutron by an atomic nucleus. That reaction is
endothermic, and the Q value is negative and equal in magnitude to the excitation energy of the final state
of the nucleus with respect to its ground state.

4.3.3 Scattering of Photons by Free Electrons


This scattering process is known as the Compton effect, to recognize its 1923 discovery by A.H. Compton.
Since the photon has zero rest mass, p = E/c and p = E  /c. Because the electron is free, the scattering is
elastic and E = E  + T . Thus, Eqs. (4.25) and (4.26) reduce to

E
E = , 0 ≤ θs ≤ π, (4.32)
1 + (E/me c2 )(1 − cos θs )

and
2me c2 E 2 cos2 θr
T = , 0 ≤ θr ≤ π/2. (4.33)
(E + me c2 )2 − E 2 cos2 θr
102 Radiation Interactions in Matter Chap. 4

Here me c2 is the rest-mass energy of the electron, 0.51099892 MeV or 8.1871 × 10−14 J. These equations are
very much simplified if expressed in terms of the dimensionless variables4 Λ = me c2 /E and τ = T /me c2 ,
namely,
Λ = 1 + Λ − cos θs , (4.34)
and
2 cos2 θr
τ= . (4.35)
(1 + Λ)2 − cos2 θr
Note that Λ ≤ Λ ≤ Λ + 2. Note too that the maximum energy transfer to initial kinetic energy of a
recoil electron is given by
T 2
= , (4.36)
E max Λ+2
which approaches unity for incident photons of very high energy. Similarly,

E Λ
= (4.37)
E Λ + 1 − cos θs

and
E Λ
= , (4.38)
E min Λ+2
which approaches unity for incident photons of very low energy. A relationship between scattering angles is
given by
cot θr = (1 + Λ−1 ) tan(θs /2) . (4.39)

4.3.4 Scattering of Neutrons by Atomic Nuclei


The scattering interaction is the most probable interaction of fast neutrons and is the mechanism relied upon
to slow these neutrons to thermal energies, at which they can be absorbed through (n, γ) reactions. There
are two distinct types of scattering processes, both of importance in fast neutron attenuation. In capture
scattering the incident neutron is absorbed by the scattering nucleus to form a compound nucleus which
subsequently decays by the emission of a neutron. If the residual nucleus is left in the ground state, the
scattering is called elastic. If the residual nucleus is left in an excited state, the scattering is called inelastic.
The other type of scattering is referred to as potential scattering. In this process, which is always elastic, the
incident neutron is scattered by the nucleus as a whole—analogous to the diffraction of the incident neutron
wave by the entire nuclear potential. Capture-scattering cross sections generally exhibit resonance behavior,
while potential scattering cross sections usually vary slowly with energy.
In all scattering processes the total energy and momentum must be conserved. Except for thermal
neutron scattering, for which the thermal motion of the target atoms may be comparable to the neutron
speed, one can properly neglect the initial kinetic energy of the scattering nucleus in the laboratory coordinate
system. Furthermore, these scattering interactions may be treated by classical mechanics, so that energy
and momentum are related by p2 = 2mE. The ratio M/m of the mass of the target nucleus to the mass of

4 Inthis book, the dimensionless variable Λ is called the reduced wavelength. Clearly it does not have units of length. Usually
in most texts the symbol for reduced wavelength is λ, but because λ is already used as the decay constant, and later is used as
actual wavelength, to avoid confusion the symbol Λ is used as a substitute. It might better be called the wave number. It may be
construed more properly as the ratio of the actual wavelength hc/E to the Compton wavelength Λc = hc/me c2 = 2.4263×10−12
m, in which h is Planck’s constant, 6.6261 × 10−34 J s. More correctly, then, Λ is the wavelength in units of the Compton
wavelength.
Sec. 4.3. Scattering Interactions 103

the neutron is so nearly equal to the atomic mass A of the target nucleus that in this book, the difference is
neglected. In the general case of inelastic scattering, Eqs. (4.24) to (4.26) reduce to (see Problem 16)
   
 1 E E QA
ωs (E, E ) = (A + 1) − (A − 1) −√ , (4.40)
2 E E EE 
in which ωs ≡ cos θs , −1 ≤ ωs ≤ +1. It follows that
√ 1  √  
E = ωs E ± E(ωs2 + A2 − 1) + A(A + 1)Q (4.41)
(A + 1)
and
AE   
T = Δ + 2 cos2
θr ± (Δ + 2 cos2 θ )2 − Δ2 ,
r (4.42)
(1 + A)2
in which
Q(1 + A)
Δ= (4.43)
AE
and 0 ≤ θr ≤√π/2.
Because E  physically must be non-negative, only the plus sign in Eqs. (4.41) and (4.42) gives meaningful
results for elastic scattering (Q = 0) and for most inelastic scattering. However, when a neutron with energy
only slightly greater than |Q| is inelastically scattered, both signs may lead to physically realistic results.
This so-called “double value” region is discussed below.

4.3.5 Threshold Energies for Neutron Inelastic Scattering


From Eq. (4.41), it is clear that for E  to be real it is necessary that
A(A + 1)Q
E≥− . (4.44)
ωs2 + A2 − 1
The least value of E allowing inelastic scatter, the threshold energy Et , corresponds to ωs = 1, namely,
A+1
Et = − Q. (4.45)
A
The energies of the first and second excited nuclear states tend to decrease as the atomic weight A
increases. Consequently, the threshold for inelastic scattering tends to decrease as the atomic mass of the
scatterer increases. The level spacings of the light elements and the magic number5 nuclides are relatively
large and hence inelastic scattering is generally less significant for such nuclides. Moreover, the odd-even
and even-odd nuclides tend to have smaller thresholds than the even-even nuclides.
It is also clear from Eq. (4.41) that for values of E just greater than Et , the scattered neutron
can appear in the forward direction, ωs > 0, with either of two distinct positive energies. The
largest
√ value of E for which this is possible—the cutoff energy Ec —is the largest value of E for which
ωs E − E(ωs2 + A2 − 1) + A(A + 1)Q ≥ 0, namely,
AQ
Ec = −
. (4.46)
A−1
For E between Et andEc , there is a maximum scattering angle, or minimum ωs , permitting real values of
E  , namely, ωs,min = 1 − A2 − QA(A + 1)/E. Discussion of the implications of dual values of E  may be
found in the works of Evans [1955] and Amaldi [1959].

5A magic number nucleus is one in which the number of neutrons or protons equals 2, 8, 20, 50, 82, or 126. When the nucleus
is magic, a particularly stable configuration of the nucleons in the nucleus is achieved analogous to closed electron shells in
atomic physics.
104 Radiation Interactions in Matter Chap. 4

scattered scattered v’c vo


neutron
v’ neutron

target v’c
v nucleus qs vc qc
vo v’
qs
incident
qr
neutron nucleus qc initial neutron
neutron
direction
center
recoil recoil
of mass
nucleus
nucleus Vr V’c

(a) (b) (c)


Figure 4.3. Conversion between laboratory and center-of-mass coordinate systems. (a) Velocities in the
laboratory system. (b) Velocities in the center-of-mass system. (c) Relationship between scattering angles
in the two systems.

4.3.6 Neutron Scattering in the Center-of-Mass System


Particle kinematics may be described and understood completely in the laboratory coordinate system used
implicitly to this point. It may therefore seem a needless complication to introduce a different coordinate
system—the center-of-mass system. Nevertheless, there are certain aspects of particle kinematics that are
greatly simplified when described in the new system. This is especially true for angular characteristics of
scattering cross sections and angular distributions of neutrons after scattering. Such distributions are more
easily and more precisely described in the center-of-mass system. For example, the angular distribution of
neutrons scattered from hydrogen atoms or, indeed, the angular distribution of billiard balls after elastic
collision is very anisotropic in the laboratory system but completely isotropic in the center-of-mass system.
Consider the scattering reaction illustrated in Fig. 4.3(a). The target nucleus is initially at rest. Prior
to scatter, the center of mass is moving to the right with velocity vo defined in such a way that the total
linear momentum mv is equal to (m + M )vo . In the center-of-mass system, Fig. 4.3(b), the center of mass is
stationary. Prior to scatter, the target atom is moving to the left with velocity vo and the incident neutron
is moving to the right with velocity vc = v − vo . The total momentum before and after scattering is zero.
Thus, products of the scattering must move in opposite directions, the neutron with velocity vc and the
recoil nucleus with velocity Vc . Figure 4.3(c) illustrates the relationship between the scattering angles in
the two systems and, as addressed in Problem 18, reveals that in terms of their cosines, where from Fig. 4.3,
ωs = cos θs , ωr = cos θr , and ωc = cos θc ,

γ + ωc
ωs =  (4.47)
1 + 2γωc + γ 2

and6

ωc = −γ(1 − ωs2 ) ± ωs 1 − γ 2 (1 − ωs2 ), (4.48)

6 Forelastic scattering, only the positive sign in Eq. (4.48) applies, with one exception. For A = 1, ωs ≥ 0, and ωc = −1 + 2ωs2 .
For inelastic scattering, the positive sign applies except in the region of dual values of E  , and then ωs > 0 and ωc is dual
valued.
Sec. 4.3. Scattering Interactions 105

in which (see Problem 20)


−1/2
vo A(A + 1)Q
γ≡ = A2 + . (4.49)
vc E
Energies after scattering are given by (see Problem 21)

1 1 √ QA
E = E(1 + α) + (1 − α)Eωc 1 + Δ + (4.50)
2 2 A+1
and  
1 √ Q
T = E − E + Q = E(1 − α) 1 − ωc 1 + Δ + , (4.51)
2 A+1
in which
2
A−1
α≡ . (4.52)
A+1
Note that E  /E always lies between the limits


√ 2 
√ 2
Emin A 1+Δ−1 Emax A 1+Δ+1
= and = . (4.53)
E 1+A E 1+A

4.3.7 Limiting Cases in Classical Mechanics of Elastic Scattering


By setting Q = 0 and E  = E − T in Eqs. (4.41) and (4.50) and using Eq. (4.27), one finds that

T 2A 4A
= (1 − ωc ) = ω2, (4.54)
E (1 + A)2 (1 + A)2 r

where A ≡ M/m. Thus,   


1 − ωc θc
ωr = = sin . (4.55)
2 2
By substituting ωc = 1 − 2ωr2 from this equation into Eq. (4.47), one finds that for the classical mechanics
of elastic scattering,
1 − [2Aωr2 /(A + 1)]
ωs =  . (4.56)
1 − [4Aωr2 /(A + 1)2 ]
Listed as follows are limiting values of scattering parameters for three cases.
Case 1: m = M . This case describes neutron-proton scattering and the scattering by stationary free
electrons of low-energy electrons or positrons. All scattering angles are possible in the center-of-mass system,
but in the laboratory system, θs and θr are limited to the range 0 to π/2.

θc θs θr E  /E T /E
0 0 π/2 1 0
π/2 π/4 π/4 1/2 1/2
π π/2 0 0 1

Case 2: m < M . This case describes electron scattering by nuclei and neutron scattering from heavier
nuclei. Scattering is possible for values of θs and θc between 0 and π but for θr only between 0 and π/2. As
A increases, θs approaches θc .
106 Radiation Interactions in Matter Chap. 4

θc θs θr E  /E T /E
0 0 π/2 1 0
π/2 tan−1 A π/4 (1 + α)/2 (1 − α)/2
π π 0 α 1−α

Case 3: m > M . This case approximately describes scattering of heavy charged particles by electrons.
Scattering is possible for 0 ≤ sin θs ≤ M/m. As M/m → 0, θs → 0.

4.3.8 Relativistic Elastic Scattering of Electrons and Heavy Charged Particles


The basic working equation follows directly from the conservation laws, Eqs. (4.24) through (4.29), namely,

2M c2 p2 c2 ωr2
T =  2 . (4.57)
M c2 + p2 c2 + m2 c4 − p2 c2 ωr2

The maximum energy is transferred to the recoil target when ωr = 1. In terms of β ≡ v/c, and in terms of
Eqs. (4.30) and (4.31),
 
β2 2M m2 c2
Tmax =  . (4.58)
1 − β 2 m2 + M 2 + [2mM/ 1 − β 2 ]

Electron-Electron Scattering
Here M = m = me . The scattered and recoil electrons are indistinguishable, so the convention is adopted
that the one with the lesser energy is identified as the recoil:
⎡ ⎤
2 2
β ⎢ 2me c ωr2 ⎥
T = ⎣  ⎦ (4.59)
1 − β2 2
1 + [1/ 1 − β 2 ] − β 2 ωr2 /(1 − β 2 )

and
 
β2 m e c2
Tmax =  = E. (4.60)
1 − β2 1 + [1/ 1 − β 2 ]

4.4 Cross Sections for Photon Interactions


For details of the mechanisms of photon interactions, the reader is referred to the standard reference works of
Heitler [1954] and Evans [1955]. For comprehensive data tabulations, the reader is referred to ANSI [1991],
Biggs and Lighthill [1972], Cullen [1994], Cullen et al. [1989], Hubbell [1969, 1982], Hubbell and Seltzer
[1995], Hubbell et al. [1975, 1979], Plechaty et al. [1975], Seltzer [1993], and Trubey et al. [1989]. Photon
energies between 10 eV and 10 MeV are important in the design and analysis of photon radiation detectors.
For this energy range, only the photoelectric effect, pair production, and Compton scattering mechanisms
of interaction are significant. Of these three, the photoelectric effect predominates at the lower photon
energies. Pair production is important only for higher-energy photons. Compton scattering predominates at
intermediate energies. In rare instances one may need to account also for coherent scattering.
Sec. 4.4. Photon Cross Sections 107

4.4.1 Thomson Cross Section for Incoherent Scattering


Incoherent scattering refers to the interaction of a photon with an individual electron, as distinguished from
the coherent interaction of a photon with all electrons of an atom. It is assumed in the discussion that
follows that the incident radiation is not polarized.
In the limit of zero photon energy, scattering of the photon by a free electron may be treated by the
classical theory of radiation. The electron in the electromagnetic field of the incident radiation vibrates
with the same frequency as that of the incident radiation, thereby giving rise to the emission of secondary
electromagnetic radiation of the same frequency. Named for discoverer of the electron, J.J. Thomson (1856–
1940) [see Thomson 1897], the total cross section per electron for such scattering is
8 2
σT = πr , (4.61)
3 e
in which re is the classical electron radius. The value of re is given by
qe2
re = , (4.62)
4πo me c2
where qe is the electronic charge, 1.6022 × 10−19 C, and o is the permittivity of free space, 8.8542 ×
10−14 F cm−1 . Thus, re = 2.8179 × 10−13 cm and σT = 6.6525 × 10−25 cm2 .
For unpolarized incident radiation, the Thomson electronic cross section per steradian for scattering at
angle θs , as in Fig. 4.2, is
dσT (θs ) 1
= re2 (1 + cos2 θs ). (4.63)
dΩs 2
Knowledge of the Thomson cross section is important for two reasons. It is the low-energy limit for the
incoherent (Compton) scattering cross section. It is also, as is evident from Eq. (4.82), the basis for computing
Rayleigh-scattering cross sections for interactions of photons coherently with atomic electrons.

4.4.2 Klein-Nishina Cross Section for Incoherent Scattering


The atomic Compton cross section for incoherent scattering may be approximated as the atomic number
times the electronic cross section for scattering by a free electron (i.e., the total Klein-Nishina cross section
σKN ), namely
σc = Z σKN . (4.64)
The differential scattering cross section per electron dσKN (Λ, θs )/dΩs was calculated by Klein and Nishina
[1929] and by Tamm [1930]. This differential scattering cross section for unpolarized photons is7
 
dσKN (Λ, θs ) 1 2 Λ2 Λ 1 + Λ − cos θs
= re + − sin θs .
2
(4.65)
dΩs 2 (1 + Λ − cos θs )2 1 + Λ − cos θs Λ
A convenient alternative form is
dσKN (E, θs ) 1
= re2 ζ[1 + ζ 2 − ζ(1 − cos2 θs )], (4.66)
dΩs 2
in which ζ ≡ E  /E = Λ/Λ is given by Eq. (4.37). This cross section is illustrated in Fig. 4.4. Note that as Λ
approaches infinity, that is, E approaches zero, ζ approaches unity and Eq. (4.66) reduces to the Thomson
formula, Eq. (4.63).

7 Although both polarized and unpolarized cases were derived, the unpolarized case is generally of more interest for radiation
detection.
108 Radiation Interactions in Matter Chap. 4

90
1.0
120 60 Primary Photon Energy
0.8 Eg = 0
Eg = 50 keV
0.6 Eg = 100 keV
150 30 Eg = 250 keV
0.4 Eg = 511 keV
Primary
Photon 0.2
Direction qs
180 0.0 0
1.0 0.8 0.6 0.4 0.2 0.0 0.2 0.4 0.6 0.8 1.0
0.2 Eg = 4 MeV
Eg = 3 MeV
0.4 Eg = 2 MeV
210 330 Eg = 1.5 MeV
0.6
Eg = 1 MeV

0.8

240 300
1.0
270

Figure 4.4. Shown is the function dσKN /dΩs divided by re2 as a function of scattering angle
θ. Notice that the number of photons scattered into a unit differential solid angle increases
in the forward direction as the primary photon energy increases.

One must be wary in interpreting Fig. 4.4. At first glance


an observer might mistakenly think that high energy pho-
tons are primarily scattered directly forward. Although the
term dσKN /dΩs increases with decreasing angle θ as energy
increases (as shown in Fig. 4.4), the total differential solid
angle defined by dΩs decreases as θ decreases (see Fig. 4.5).
Dq2 This change in solid angle with angle θ is defined by
Dq1
dΩs
DW1 = 2π sin θs , (4.67)
DW2
dθs

which clearly increases as θs approaches 90o . Further, when


θs = 0, dΩs /dθs = 0. Hence, the density of photons scattering
into dΩs increases with decreasing θ, but the total probability
of photons scattering into the differential solid angle, dΩs , is
proportional to the product of the differential solid angle and
Figure 4.5. For equal Δθi , the solid angle ΔΩi
increases as θ increases from 0 to π/2.
the density of photons scattered into a unit solid angle about
angle θ, namely the differential scattering cross section.
The distribution of photons scattered per unit polar angle θs is quite different than dσKN /dΩs . Multiplying
Eq. (4.66) by Eq. (4.67) yields the probability of scattering a photon of initial energy E through angle θs ,
namely
dσKN (E, θs ) dσKN (E, θs ) dΩs
= = πre2 ζ[1 + ζ 2 − ζ(1 − cos2 θs )] sin θs . (4.68)
dθs dΩs dθs
Sec. 4.4. Photon Cross Sections 109

This cross section is plotted in Fig. 4.6. 3.5 Primary Photon


Notice that there is still a preference for for- Energies (Eg) Eg = 0 keV
ward scattering with increasing photon en- 3.0
ergy; however, the highest cross section is 50 keV
2.5
no longer at θs = 0o , and it changes as
100 keV
a function of E. Notice also, quite unlike

dq re2
dsKN 1
2.0
Fig. 4.4, which shows the density of photons
scattering into dΩs , that the highest differ- 250 keV
1.5
ential cross section in Fig. 4.6 for low energy 511 keV
photon (Thomson) scattering is at scattering 1.0 1 MeV
angles of 55o and 125o . 1.5 MeV
A related quantity is the energy scatter- 0.5 2 MeV
3 MeV
ing differential cross section, 4 MeV
0.0
dσKNe (E, θs ) E  dσKN (E, θs ) 180 160 140 120 100 80 60 40 20 0
≡ =
dΩs E dΩs Photon Scattering Angle (q)
Z 2 2
r ζ [1 + ζ 2 − ζ(1 − cos2 θs )]. (4.69) Figure 4.6. Shown is dσKN /dθs divided by re2 as a function of scatter-
2 e ing angle θs . Notice that the number of photons scattered into angle
θs increases towards the forward direction (approaching θs = 0) as the
The total Compton cross section per primary photon energy increases; however, dσKN /dθs approaches zero
atom, based on the free-electron approxima- as θs goes to zero for all photon energies.
tion, is obtained from Eq. (4.65) by integra-
tion over all directions.
 +1
dσKN (Λ, θs )
σC (Λ) = ZσKN (Λ) = 2πZ d(cos θs )
−1 dΩs
 
2 2(1 + 9Λ + 8Λ2 + 2Λ3 )
= πZre2 Λ (1 − 2Λ − 2Λ2 ) ln 1 + + . (4.70)
Λ (Λ + 2)2

Other Differential Compton Cross Sections


The cross section, per unit wavelength, for scattering of a photon into wavelength Λ without regard to angle
is, from Eq. (4.69),8
 2    
dσC (Λ, Λ ) dσKN (Λ, Λ ) Λ Λ Λ
= Z = Zπ re2 + + (Λ − Λ)(Λ − Λ − 2) . (4.71)
dΛ dΛ Λ Λ Λ

A related quantity is the cross section, per unit recoil electron energy, for creating a recoil electron with
energy T . Here it is convenient to use the ratio τ ≡ T /me c2 . Because 1/Λ−1/Λ = τ , dΛ /dτ = Λ2 (1−Λτ )−2 .
Thus, σKN (Λ, τ ) = σKN (Λ, Λ )dΛ /dτ , or

dσC (Λ, τ ) (Λ2 τ )(Λ2 τ + 2Λτ − 2)


= πZ re2 Λ2 (1 − Λτ ) + (1 − Λτ )−1 + . (4.72)
dτ (1 − Λτ )2

Energy Spectrum of Recoil Electrons


Unlike shielding analyses in which the more penetrating scattered photon is of primary interest, for energy
spectroscopy detectors it is the energy spectrum of the recoil secondary electron produced in Compton

8 Note that σ(Λ, θs ) = −σ(Λ, Λ ) × dΛ /dΩs and that dΛ /dΩs = (1/2π) dΛ /dωs = −1/2π.
110 Radiation Interactions in Matter Chap. 4

scattering that is of primary interest. The energy of the secondary electron is simply T = E − E  or from
Eq. (4.37), in terms of dimensionless quantities,
1 1 1 − cos θs
τ= −  = . (4.73)
Λ Λ Λ(1 + Λ − cos θs )

Because Λ = me c2 /E and τ = T /me c2 , this relation reduces to

E(1 − cos θs )
T = . (4.74)
me c2 /E + (1 − cos θs )

The Compton recoil electron energy function described in Eq. (4.73) is plotted in Fig. 4.7, which clearly
shows that the majority of energy is lost to the Compton recoil electrons for angles θs greater than 90o .
This result means that, although more photons are generally scattered in the forward direction, as shown in
Fig. 4.6, the energy transferred to the Compton recoil electrons is distributed over a wider range of energies.
Conversely, fewer photons are scattered from 90o –180o; however, the energy transferred to the Compton
recoil electrons is distributed over a smaller range of energies as T approaches the maximum energy defined
by Eq. (4.36).
Also of importance is the probability the recoil electron has a particular value. Let g(Λ, T ) be the
probability that the recoil electron has an energy, per unit energy about T . This probability density function
can be computed as
dτ 1 dσC (Λ, τ )/dτ
g(Λ, T ) = g(Λ, τ ) = . (4.75)
dT m e c2 σC (Λ)
This expression is readily evaluated from Eqs. (4.70) and (4.72) and is shown in Fig. 4.8.
Compton Energy-Absorption and Energy-Scattering Cross Sections
The mean fraction of the photon energy transferred to the recoil electron is designated as fC and the Compton
energy-absorption cross section9 per electron is defined as

σCa (Λ) ≡ fC σC (Λ). (4.76)

The factor fC is the weighted average of T /E = Λτ , namely,


 2/[Λ(Λ+2)]
1
fC = dτ Λτ σC (Λ, τ ). (4.77)
σC (Λ) 0

The energy-scattering cross section is the product of the total cross section and the mean fraction of the
photon energy retained by the scattered photon:

σCe (Λ) = (1 − fC ) σC (Λ). (4.78)

It is evident from the definition of fC that the factor (1 − fC ) can be evaluated as the mean value of
E  /E = Λ/Λ , namely,
 Λ+2
1 Λ
1 − fC = dΛ  σC (Λ, Λ ). (4.79)
σC (Λ) Λ Λ

9 The Compton energy absorption cross section thus defined is not a true cross section for photon absorption since, in the
interaction, a scattered photon always results. Rather, it is an effective energy absorption cross section with respect to the
incident photon energy such that the product E(μCa /ρ)φ is the rate per unit mass at which energy is transferred to initial
kinetic energy of Compton recoil electrons.
Sec. 4.4. Photon Cross Sections 111

4.0
Primary Photon 4 MeV
3.5 Energies
Scattered Compton Recoil
Electron Energy (MeV)

3.0
3 MeV
2.5

2.0
2 MeV
1.5
1.5 MeV
1.0
1 MeV
0.5 511 keV
0.0
0 20 40 60 80 100 120 140 160 180
Angle (q) of Scattered Photon

Figure 4.7. The Compton recoil electron energy as a function of primary


photon energy and scattered photon angle θs . Notice that the change in
Compton electron energy is small for photon scattering angles above 90o .

Figure 4.8. The Compton recoil electron spectrum as a function of Compton


electron energy.
112 Radiation Interactions in Matter Chap. 4

4.4.3 Incoherent Scattering Cross Sections for Bound Electrons


The equations for scattering from free electrons break down when the kinetic energy of the recoil electron
would be comparable to its binding energy in the atom. Thus, binding effects might be thought to be an
important consideration for the attenuation of low-energy photons in media of high atomic number. For ex-
ample, the binding energy of K-shell electrons in lead is 88 keV. However, under these same circumstances,
cross sections for the photoelectric interaction of photons greatly exceed incoherent scattering cross sections.
Radiation attenuation in this energy region is dominated by photoelectric interactions, and in most atten-
uation calculations, the neglect of electron binding effects on incoherent scattering causes negligible error.
Corrections for electron binding and related data are available in the literature [e.g., Storm and Israel 1967;
Biggs and Lighthill 1972; Plechaty et al. 1975; Hubbell 1982; Trubey et al. 1989]. The total atomic cross
section for incoherent scattering by bound electrons is given by
 +1
dσKN (Λ, θs )
σincoh (Λ) = 2π d(cos θs ) S(x, Z) , (4.80)
−1 dΩs

in which S(x, Z) is the incoherent scattering function [Hubbell et al. 1975] and x is the momentum-transfer
parameter, given approximately by
E
x= sin(θs /2). (4.81)
hc
Figure 4.9 shows the relative importance, in lead, of electron binding effects by comparing photoelectric cross
sections with those for incoherent scattering from both free and bound electrons. As is apparent, S(x, Z) is
very small for low-energy photons and approaches Z as photon energy increases.

4.4.4 Coherent (Rayleigh) Scattering


In competition with the incoherent scattering of photons by individual electrons is coherent scattering by the
electrons of an atom collectively. Since the recoil momentum in the Rayleigh interaction is taken up by the
atom as a whole, the energy loss of the gamma photon is slight and the scattering angle small. For example,
for 1-MeV photons scattering coherently from iron atoms, 75% of the photons are scattered within a cone of
less than 4◦ half-angle [Hubbell 1969]. As is apparent from Fig. 4.9, coherent scattering cross sections may
greatly exceed incoherent scattering cross sections, especially for low-energy photons and high-Z materials.
However, because of the minimal effect on photon energy and direction, and because the coherent scattering
cross section is so much less than the cross section for the photoelectric effect, it is common practice to
ignore Rayleigh scattering in the design of many photon detectors, especially when electron binding effects
mentioned in the preceding section are ignored. Named for the 4th Lord Rayleigh, R.J. Strutt (1875–1947),
the scattering cross section per atom is

dσR (E, θs ) 1
= re2 (1 + cos2 θs )[F (x, Z)]2 , (4.82)
dΩs 2

in which F (x, Z) is the atomic form factor, and the momentum-transfer parameter x is given by Eq. (4.81).
Form factors are tabulated by Hubbell and Overbø [1979]. As E approaches zero, F (x, Z) approaches Z and
σR varies as Z 2 . Effects of coherent scattering are addressed in detail by Trubey and Harima [1987] and
data are available in an ANSI standard [1991].

4.4.5 Photoelectric Effect


In the photoelectric effect, a photon interacts with an entire atom, resulting in the emission of a photoelectron,
usually from the K shell of the atom. Although the difference between the photon energy E and the electron
Sec. 4.4. Photon Cross Sections 113

Figure 4.9. Comparison of scattering, photoelectric-effect, and pair-production cross sections for
photon interactions in lead.

binding energy Eb is distributed between the electron and the recoil atom, virtually all of that energy is
carried as kinetic energy of the photoelectron because of the comparatively small electron mass. Thus,
T = E − Eb .
K-shell binding energies Ek vary from 13.6 eV for hydrogen to 7.11 keV for iron, 88 keV for lead, and
116 keV for uranium. As the photon energy drops below Ek , the cross section drops discontinuously. As
E decreases further, the cross section increases until the first L edge is reached, at which energy the cross
section drops again, then rises once more, and so on for the remaining edges. These “edges” for lead are
readily apparent in Fig. 4.9. The cross section varies as E −n , where n  3 for energies less than about 150
keV and n  1 for energies greater than about 5 MeV. The atomic cross section varies as Z m , where m
varies from about 4 at E = 100 keV to 4.6 at E = 3 MeV. As a very crude approximation in the energy
region for which the photoelectric effect is dominant,
Z4
σph (E) ∝ . (4.83)
E3
Although it is true that for light nuclei, K-shell electrons are responsible for almost all photoelectric inter-
actions, such interactions are normally much less important than incoherent scattering. As a general rule,
about 80% of photoelectric interactions with heavy nuclei result in ejection of a K-shell electron. Conse-
quently, the approximation is often made for heavy nuclei that the total photoelectric cross section is 1.25
times the cross section for K-shell electrons.
114 Radiation Interactions in Matter Chap. 4

As the vacancy left by the photoelectron is filled by an electron from an outer shell, either fluorescence
x rays or Auger electrons10 may be emitted. The probability of x-ray emission is given by the fluorescent
yield. For the K shell, fluorescent yields vary from 0.005 for Z = 8 to 0.965 for Z = 90. Although x rays of
various energies may be emitted, the approximation is often made that only one x ray or Auger electron is
emitted, with energy equal to the binding energy of the photoelectron.



 

















     

    

Figure 4.10. Differential pair-production cross section in iron, in the form of the mass
interaction coefficient. The function μ(E, T ) dT is the probability per unit distance of travel
that a photon of energy E experiences a pair-production interaction in which a product
electron has kinetic energy between T and T + dT . Data derived using the PEGS4 Code
[Nelson, Hirayama, and Rogers 1985].

4.4.6 Pair Production


In this process, the incident photon is completely absorbed and in its place appears a positron-electron pair.
The phenomenon is induced by the strong electric field in the vicinity of the nucleus and has a photon
threshold energy of 2me c2 (= 1.02 MeV). In the nuclear pair production process, the nucleus acquires
indeterminate momentum but negligible kinetic energy. Thus,

T+ + T− = E − 2me c2 , (4.84)

in which T+ and T− are the kinetic energies of the positron and electron, respectively. To a first approxi-
mation, the total atomic pair production cross section varies as Z 2 . The cross section increases with photon
energy, approaching a constant value at high energy. As illustrated in Fig. 4.10, the resulting electron and

10 If
an electron in an outer shell, say Y, makes a transition to a vacancy in an inner shell, say X, an x ray may be emitted with
energy equal to the difference in binding energy between the two shells. Alternatively, an electron in some other shell, say
Y , which may be the same as Y, may be emitted with energy equal to the binding energy of the electron in shell X less the
sum of the binding energies of electrons in shells Y and Y . This electron is called an Auger electron. If an electron makes a
transition from one subshell to a vacancy in another subshell of the same shell, the small difference in binding energies may
be transferred to an outer-shell electron, in this case called a Coster-Kronig electron.
Sec. 4.4. Photon Cross Sections 115

positron are widely distributed in energy. Both have directions not far from the original direction of the
photon but separated by π radians in azimuth about the photon direction. As an approximation, the angles
ϑ with respect to the photon direction are me c2 /E radians.
Far less likely than nuclear pair production,
a photon of sufficient energy can interact in the
electric field of an orbital electron producing
an electron-positron pair and a recoil orbital
electron. This electron pair production is re-
ferred to as triplet production and is, except for
the lightest nuclei, a small fraction of the to-
tal pair production events (see Fig. 4.11). It
can be shown that because of the constraints
of conservation of energy and momentum the
threshold photon energy for triplet production is
4me c2  2.044 MeV, twice that for pair produc-
tion. The photon energy less the energy equiva-
lent of four electron masses is shared as kinetic
energy among the positron and the two elec-
Figure 4.11. Ratio of the triplet to total pair production cross sec-
trons, namely tions as a function of the Z-number of the nuclide for three incident
photon energies.
Te+ + T1e− + T2e− = E − 4me c2 . (4.85)
The fate of the positron produced in pair production is annihilation with an ambient electron, generally
after slowing to practically zero kinetic energy. This annihilation process results in the creation of two
photons moving in opposite directions (to conserve the near zero linear momentum of the slowed electron
and positron), each with energy me c2 .

4.4.7 Photon Interactions—Minor Effects


Discussed above are the photon interaction mechanisms that are important for radiation detection. Photons
can interact with matter in several other ways, but are relatively unimportant for most detector designs.
In 1933 Max Delbrück predicted that high energy photons could be scattered in the Coulombic field
near a nucleus as a result of the polarization in the vacuum produced by this field. In this process the
incident photon is most often scattered coherently by a virtual electron-positron pair in the field, resulting
in little change in direction or loss of energy. This predicted scattering mechanism was finally confirmed
experimentally only 20 years later.
Another photon scattering mechanism is that of nuclear resonance scattering. In this process an incident
photon can be absorbed by a nucleus placing the nucleus in an excited nuclear state. Because these states
have very short lifetimes (typically ps), the energy of the incident photon must, consequently, almost exactly
match the nuclear energy level (recall the uncertainty principle ΔtΔE ≤ h/(2π)). The excited nuclear state
decays, almost always by electric dipole transitions, to lower nuclear states emitting a cascade of gamma
rays isotropically, analogous to the fluorescence x-ray cascades produced by the photoelectric effect.
Another very minor scattering process is that of nuclear Rayleigh scattering in which the nucleons scatter
an incident photon coherently just as in Rayleigh scattering from all the orbital electrons. However, this is
an extremely minor phenomenon, again with little change in direction or energy loss. These minor scattering
mechanisms are reviewed by Kane et al. [1986].
At higher energies (5-50 MeV), photons can cause (γ, n) reactions and at even higher energies they can
result in meson production. Such phenomena are of importance only in the design of detectors for high
energy physics research.
116 Radiation Interactions in Matter Chap. 4

4.4.8 Photon Attenuation Coefficients


The photon linear attenuation coefficient
μ is, in the limit of small path lengths,
the probability per unit distance of travel
that a gamma photon undergoes any sig-
nificant interaction. Thus, for a specified
medium,
μ/ρ

μ(E) = N [σc (E) + σph (E) + σpp (E)] ,


(4.86)
in which N = ρNa /A is the atom den-
sity. Note that Rayleigh scattering and
other minor effects are specifically ex-
cluded from this definition.11 More com-
mon in data presentation is the mass in-
teraction coefficient
μ Na
= [σc (E) + σph (E) + σpp (E)]
ρ A
μc μph μpp
= + + , (4.87)
ρ ρ ρ
Figure 4.12. Mass attenuation coefficients as a function of photon
in which Na is Avogadro’s number. It
energy for all the elements. Notice the smooth variation of μ/ρ with
is important to note that the mass inter-
energy and the atomic number Z, except for the discontinuities at the
edge energies. action coefficients are independent of the
mass density ρ of the material, and it is for this reason that μ/ρ rather than μ values are usually tabulated.
The variation of μ/ρ with energy for all the elements is shown in Fig. 4.12.

4.5 Neutron Interactions


The interaction processes of neutrons with matter are fundamentally different from those for the interactions
of photons. Whereas photons interact, more often, with the atomic electrons, neutrons interact essentially
only with the atomic nucleus. Although neutron-electron interactions do occur, this type of interaction is
highly improbable and therefore negligible when compared to the neutron-nucleus interactions. The cross
sections that describe the various neutron interactions are also very unlike those for photons. Neutron cross
sections not only can vary rapidly with the incident neutron energy, but also can vary erratically from one
element to another and even between isotopes of the same element. The description of the interaction of
a neutron with a nucleus involves complex interactions between all the nucleons in the nucleus and the
incident neutron, and consequently fundamental theories which can be used to predict neutron cross-section
variations in any accurate way are still lacking. As a result, all cross-section data are empirical in nature,
with little guidance available for interpolation between different energies or isotopes.
Over the years, many compilations of neutron cross sections have been generated, and the more extensive,
such as the Evaluated Nuclear Data Files (ENDF) [Kinsey 1979; Rose and Dunford 1991], contain so much
information that digital computers are used almost exclusively to process these cross-section libraries to
extract cross sections or data for a particular neutron interaction. Even with the large amount of cross-
section information available for neutrons, there are still energy regions and special interactions for which

11 When referring to data tables in other publications, the reader should be aware that occasionally Rayleigh scattering and
incoherent scattering are included.
Sec. 4.5. Neutron Interactions 117

the cross sections are poorly known. For example, cross sections for interactions which produce energetic
secondary photons or charged particles are of concern in radiation detection and often still are not known with
an accuracy sufficient to perform satisfactory analyses of neutron detectors that rely on such interactions.

4.5.1 Classification of Types of Interactions


There are many possible neutron-nuclear interactions, only some of which are of concern in radiation-
protection calculations. Ultra-high-energy interactions can produce many and varied secondary particles;
however, the energies required for such reactions are usually well above the neutron energies commonly
encountered, and therefore such interactions can be neglected here. Similarly, for low-energy neutrons many
complex neutron interactions are possible—Bragg scattering from crystal planes, phonon excitation in a
crystal, coherent scattering from molecules, and so on—none of which is of particular importance in the
design of many neutron detectors. The neutron reactions of principal importance are those that produce
various secondary radiations that, in turn, deposit energy in the active medium of a radiation detector.
The total cross section, which is the sum of cross sections for all possible interactions, gives a measure
of the probability that a neutron of a certain energy interacts in some manner with the medium through
which the neutrons are traveling. The components of the total cross section for absorption and scattering
interactions are usually of primary concern. Nonetheless, when the total cross section is large, the probability
of some type of interaction is great and thus the total cross section, which is the most easily measured and
the most widely reported, gives at least an indication of the neutron energy regions over which one must
investigate the neutron interactions in greater detail.
The total cross sections, although they vary from nuclide to nuclide and with the incident neutron energy,
have certain common features. For the sake of classification, the nuclides are usually divided into three broad
categories: light nuclei, with mass number < ∼ 25; intermediate nuclei; and heavy nuclei, with mass number
> 150. Example total cross sections for each category are shown in Figs. 4.13 through 4.15.

For light nuclei and some magic number nuclei the cross section at low energies (< 1 keV) often varies as
σ2
σt = σ1 + √ , (4.88)
E
where E is the neutron energy, σ1 and σ2 are constants, and the two terms on the right-hand side represent
the elastic scattering and the radiative capture (or absorption) reactions, respectively. For solids at energies
less than about 0.01 eV, there may be Bragg cutoffs representing energies below which coherent scattering
from the various crystalline planes of the material is no longer possible. These cutoffs are not shown in
Figs. 4.13 through 4.15. At energies greater than about 0.1 eV, the cross sections are usually slowly varying
and “smooth” up to the MeV energy range, at which energies fairly wide (keV to MeV) resonances appear.
Of all the nuclides, only hydrogen and its isotope deuterium exhibit no resonances. For both isotopes,
the cross sections above 1 eV are almost constant up to the MeV region, above which they decrease with
increasing energy.
For heavy nuclei, as√ illustrated in Fig. 4.15, the total cross section, unless masked by a low-energy
resonance, exhibits a 1/ E behavior at low energies and usually a Bragg cutoff (not shown). The resonances
appear at much lower energies than for the light nuclei (usually in the eV region) and have very narrow widths
(1 eV or less) with large peak values. Above a few keV the resonances are so close together and so narrow
that they cannot be resolved and the cross sections appear to be smooth except for a few broad resonances.
Finally, the intermediate nuclei, as would be expected, are of intermediate character between the light and
heavy nuclei, with resonances in the region from 100 eV to several keV. The resonances are not as high or
as narrow as for the heavy nuclei.
Because neutrons are invariably born with high energies (100 keV – 10 MeV), neutron radiation fields
almost always contain a spectrum of neutrons ranging from thermal energies to high energy. As neutrons
118 Radiation Interactions in Matter Chap. 4

Figure 4.13. Total neutron cross section for aluminum computed using NJOY-processed
ENDF/B (version V) data.

scatter they lose energy and, unless they are absorbing while they slow down, they eventually come into
thermal equilibrium with the ambient medium. Detector materials that have large thermal absorption
cross sections for producing charged reaction products are typically used to detect thermal neutrons. Three
commonly used isotopes are 3 He, 10 B, and 6 Li, all having large thermal σ(n,p) , σ(n,α) , and σ(n,t) cross sections,
respectively. These cross sections are shown in Fig. 4.16. Another charged-particle producing reaction that
is useful for detecting thermal neutrons is the fission reaction.
Alternatively, one could use (n, γ) absorption reactions and use a photon detector. If the result of such
a reaction produces a radioactive isotope, then detectors for the radiation emitted by the isotope’s decay
can be used to infer the presence of neutrons. However, the absorption cross sections at all energies, except
Sec. 4.5. Neutron Interactions 119

Figure 4.14. Total neutron cross section for iron computed using NJOY-processed ENDF/B
(version V) data.

thermal energies, for all nuclides are usually small compared to other reactions. Over the fission-neutron
energy spectrum, the (n, γ) reaction cross sections seldom exceed 200 mb for the heavy elements, and for
the lighter elements this cross section is considerably smaller. Only for thermal neutrons and a few isolated
absorption resonances in the keV region for heavy elements is the (n, γ) reaction important.
In the high energy region, by far the most important neutron interaction is the scattering process.
Generally, elastic scattering is more important, although, when the neutron energy somewhat exceeds the
energy level of the first excited state of the scattering nucleus, inelastic scattering becomes possible. The
recoil energy of the scattering nucleus can be measured and used to infer the energy distribution of incident
neutrons. Also in the MeV region the (n, α) reaction cross sections for Be, N, and O are appreciable fractions
120 Radiation Interactions in Matter Chap. 4

Figure 4.15. Total neutron cross section for uranium computed using NJOY-processed ENDF/B
(version V) data. Above 4 keV the resonances are no longer resolved and only the average cross-
section behavior is shown.
Sec. 4.5. Neutron Interactions 121

Figure 4.16. Total neutron cross sections for 3 He, 10 B, and 6 Li (heavy lines)
and the (n, p), (n, α), and (n, t) cross sections (light lines), respectively.

of the total cross sections and may exceed the inelastic scattering contributions. This situation is probably
true for most light elements, although only partial data are available. For heavy and intermediate nuclei
the charged-particle emission interactions are at most a few percent of the total inelastic interaction cross
section and hence are usually ignored.
4.5.2 Thermal Neutron Interactions
As neutrons slow through scattering, their speeds become comparable to those of the ambient atoms in
thermal motion. In this case it is important to account for the motion of both the neutrons and the interacting
nuclei. In the following treatment, it is assumed that neutrons interact with only a single atom at a time
(unlike, for example, Bragg scattering) so that interactions can be described by microscopic cross sections.
Let n(v)dv and N (V)dV be the number density at some point of interest of, respectively, the neutrons
with laboratory velocities in dv about v and the atoms with laboratory velocities in dV about V. Neutrons
and nuclei thus approach each other with a relative velocity vr = v − V. Now consider a coordinate system
in which the atomic nuclei are at rest, so that the neutrons approach the nuclei with the relative velocity vr .
Thus, from the nuclei’s perspective, the neutrons appear as a beam with intensity dI = n(v)vr dv, where
vr = |vr |. These neutrons cause interactions of type i at a rate of

dFi = n(v)N (V)σi (vr )vr dv dV (4.89)

interactions cm−3 s−1 . The total interaction rate density for neutrons and nuclei of all speeds is thus [Lamarsh
1966]

Fi = n(v)N (V)σi (vr )vr dv dV, (4.90)

where the integration is over the six components of v and V. Below several special cases are considered.
More general cases are considered by Meghreblian and Holmes [1960].
122 Radiation Interactions in Matter Chap. 4

1/v Absorption
Consider now the case of thermal neutron absorption (capture or fission). In the thermal energy range σa (v)
varies as 1/v, so that
vro
σa (vr ) = σa (vvo ), (4.91)
vr
where vro is an arbitrary reference speed. Substitution of this result into Eq. (4.90) gives

Fa = vro σa (vro ) n(v)N (V) dv dV = N σa (vro )nvro , (4.92)

where N and n are, respectively, the atomic and neutron number densities. This astounding result shows
that the absorption rate of a 1/v absorber is a constant that is independent of the velocity distributions
of either the neutrons or atoms! Here Fa depends only on a single arbitrary relative speed vro between
the neutron and nucleus. McGregor and Shultis [2011] show the benefit of this result for neutron detector
calibrations. One could also view all the nuclei at rest and treat vro as an arbitrary laboratory speed of the
neutron. Thus, the absorption rate density can be calculated as

Fa = Σa (Eo )φo (4.93)

where φo = nvo with vo an arbitrary laboratory speed and Eo is the corresponding energy. Typically, vo
is taken as 2200 m/s so that Eo = 0.0253 eV, the most probable energy of a Maxwellian distribution at
To = 293.61 K. Here φo = nvo is the “2200-m/s flux”, the flux that would result if all thermal neutrons were
to travel at 2200 m/s.
Non-1/v Absorption
The absorption cross section of some nuclei, particularly those heavy nuclei with resonances just above
the thermal region, deviates significantly from the ideal 1/v behavior. However, for such heavy nuclei the
center-of-mass and laboratory coordinate systems are nearly the same, so that vr in Eq. (4.90) equals the
laboratory speed v of the neutrons. Equation (4.90) becomes
 
Fa = n(v)N (V)σ(v)v dv dV = N n(v)σ(v)v dv. (4.94)

Because n(v) dv = n(E) dE where E is the laboratory neutron energy, Eq. (4.94) transforms to
 
Fa = N n(E)σa (E)v(E) dE = Σa (E)φ(E) dE, (4.95)

where the integration is over all thermal energies.


In many instances the energy dependence of thermal neutrons is well approximated by a Maxwellian
distribution with an effective neutron temperature T , i.e., by

2πn 2
φM (E, T ) = E exp[−E/kT ], (4.96)
(πkT )3/2 mn

where n is the neutron density, mn is the neutron mass, k is Boltzmann’s constant (k = 8.617 343 × 10−5 eV
K−1 ).
In this case Eq. (4.95) can be numerically evaluated to give

Fa = ga (T )Σa (Eo )φo = Σa φt , (4.97)


Sec. 4.5. Neutron Interactions 123

where the total thermal flux


 ∼5kT  ∞
φt = φ(E) dE  φM (E, T ) dE, (4.98)
0 0

and the thermal-averaged macroscopic absorption cross section is


√  1/2
π To
Σa = ga (T ) Σa (Eo ). (4.99)
2 T

In this result, the Westcott non-1/v factor ga (T ) accounts for deviations


√ from the 1/v behavior of absorption
cross sections in the thermal energy region.12 If σa (E)  1/ E, then ga (T ) = 1. Finally, the relation
between the thermal flux φt and the fictitious 2200-m/s flux is obtained from Eqs. (4.97) and (4.99) as
 1/2
2 T
φt = √ φo . (4.100)
π To

The result for the absorption rate density of Eq. (4.95) is also obtained for light nuclei with non-1/v
behavior and for which the center-of-mass and laboratory systems are not equal, provided both the neutrons
and atoms have Maxwellian distributions of energy with the same temperature [Lamarsh 1966].
Scattering Interaction Rate
Scattering cross sections at thermal energies (always elastic) are usually nearly constant, i.e., Σs (E) 
Σs (Eo ). The scattering interaction rate density is given by

Fs = Σs (E)φ(E) dE. (4.101)

If Σs (E) = Σs (Eo ), then clearly Fs = Σs (Eo )φt . Sometimes Σ(E) is not quite constant. In this case,
Eq. (4.101) is integrated numerically after assuming a Maxwellian for φ(E) to give, in analogy to Eq. (4.97),

Fs = gs (T )Σs (Eo )φo = Σs φt , (4.102)

where the thermal averaged scattering cross section is


√  1/2
π To
Σs = gs (T ) Σs (Eo ). (4.103)
2 T

For the case Σs (E) = Σs (Eo ), gs (T ) = 2/ π  1.1283, a result seen in most of the scattering cross sections
listed in Appendix B, Table B.1.

4.5.3 Neutron Differential Scattering Cross Sections


The differential scattering cross section σs (E, θ) is sometimes reported in cross-section libraries in terms of
ωc , the cosine of the scattering angle in the center-of-mass coordinate system. This is done because, in the
center-of-mass system, scattering of low- and intermediate-energy neutrons is nearly isotropic, that is,
dσs (E, ωc ) σs (E)
 . (4.104)
dΩc 4π

12 Westcott used a more general form to account also for epithermal neutron absorption. See Westcott [1955].
124 Radiation Interactions in Matter Chap. 4

In fact, for hydrogen, the scattering in the center-of-mass system is isotropic for energies up to about 30 MeV.
Generally, the heavier the nuclide, the lower is the energy above which elastic scattering becomes anisotropic.
The differential scattering cross section is thus well represented by a low-order Legendre polynomial expansion
in the form
σs (E) 
N
dσs (E, ωc )
 (2n + 1)fn (E)Pn (ωc ). (4.105)
dΩc 4π n=0

Cross-section data may be tabulated in terms of the expansion coefficients fn (E). Because of the way that
Eq. (4.105) is formulated, f0 is always equal to 1. The order of the expansion seldom exceeds N = 8.
Few data are available on the angular distributions of inelastically scattering neutrons. When only one or
two levels are involved, the scattering may be anisotropic; however, it has generally been found that it is
a good approximation to assume that the inelastically scattered neutrons are emitted isotropically in the
center-of-mass system. This is particularly true when multiple levels are involved in the inelastic process.
The potential scattering of fast neutrons is never isotropic but is highly peaked in the forward directions. In
fact, the angular distribution can exhibit several maxima as the scattering angle varies.
The relation between the laboratory and center-of-mass scattering angular distributions may be obtained
from a formal change of independent variable or from recognition that the probability of scattering into
corresponding differential solid angles dΩs = 2π dωs and dΩc = 2π dωc must be the same, that is,13

dσs (E, ωs ) dσs (E, ωc )


dωs = dωc . (4.106)
dΩs dΩc

Transformations between the two systems make use of Eqs. (4.47) and (4.48) as well as the interrelationship

dωc± (1 + 2γωc± + γ 2 )3/2 1 − γ 2 (1 − 2ωs2 )


=± ± = 2γωs ± . (4.107)
dωs 1 + γωc [1 − γ 2 (1 − ωs2 )]1/2

For elastic scattering and for inelastic scattering with single values of E  , only the positive sign in this
equation applies, and there is only a single value of ωc . However, for inelastic scattering with dual values of
E  , there are two values of ωc , as indicated in Eq. (4.48). The positive signs in Eqs. (4.48) and (4.107) are
associated with ωc+ , and the negative signs with ωc− .

4.5.4 Average Energy Transfer in Neutron Scattering


Here it is necessary to be very careful in distinguishing between the kinetic energy lost by the neutron
and the kinetic energy gained by the recoil atom, for the two are not the same when the scattering is
inelastic. Knowledge of the energy lost by the neutron is important in the examination of neutron moderation.
Knowledge of the energy gained by the recoil atom is important in dosimetry. The mean fraction of the
energy E lost is described as 1 − E  /E, and the mean fraction of E transferred to the recoil atom as T /E.
The two are related by T  = E − E   + Q.
The mean fraction of energy transferred E  /E may be determined based on [dσs (E, E  )/dE  ] dE  /σs (E)
being the probability that a neutron of energy E leaves a scattering interaction with energy between E  and
E  + dE  . Thus,
 Emax

E   1 E  dσs (E, E  )
= dE  , (4.108)
E σs (E) Emin
 E dE 

13 It
should be noted that following standard usage, σs (E, ωc ) and σs (E, ωs ) are different functions even though they carry the
same symbol, σs .
Sec. 4.5. Neutron Interactions 125

Table 4.1. Average fraction 1 − E  /E of neutron energy lost in center-of-


mass scattering interactions. Note that Δ = Q(A + 1)/AE and that T  /E =
1 − E  /E + Q/E.

Isotropic scatter Anisotropic scatter

1−α 1−α
Elastic scatter [1 − f1 (E)]
2 2

1−α A 1−α A √
Inelastic scatter 1− Δ 1 − Δ − f1 (E) 1 + Δ
2 2 2 2

in which the limits are given in Eqs. (4.53). Scattering into a particular range of energies requires scattering
within an associated range of directions, that is, [dσs (E, E  )/dE  ] dE  = 2π[dσs (E, ωc )/dΩc ] dωc . Thus, from
Eq. (4.50), with Δ = Q(1 + A)/AE,

dσs (E, E  ) 4π dσs (E, ωc )


= √ . (4.109)
dE  (1 − α)E 1 + Δ dΩc

The determination of E  /E may be accomplished more simply by using the angular distribution of the
cross section directly, that is,
 +1
E   2π E  dσs (E, ωc )
= dωc , (4.110)
E σs (E) −1 E dΩc
where the ratio E  /E is given in Eq. (4.50), and by using the Legendre expansion of Eq. (4.105) for
dσs (E, ωc )/dΩc .
Evaluation of energy transfer for several cases of neutron scattering is summarized in Table 4.1. In
this table f1 is the first order Legendre expansion coefficient of Eq. (4.105). Notice that as A increases,
α approaches unity, and the average energy loss in elastic scattering approaches zero. Only by inelastic
scattering can appreciable energy losses be realized. Although for hydrogen the average energy loss is one-
half of the initial energy, the total scattering cross section σs (E) declines with increasing energy in the
MeV energy region and hydrogen scattering events become relatively improbable. For this reason inelastic
scattering by heavy nuclides plays a crucial role in the slowing of fast neutrons.
The energy of the recoil nucleus from a scattering event caused by a fast neutron is quickly dissipated
in solids or liquids, and hence for all practical purposes the recoil energy can be assumed to be deposited
locally. For example, a 5-MeV proton travels at most 0.5 mm in aluminum. Heavier recoiling nuclei are
stopped in much shorter distances. Only for the case of neutron scattering in a gas does one have to be
concerned with the travel of the recoil atoms and then only if very detailed calculations are required. The
energy distribution of the recoil nuclei is usually of great interest in radiation detection and dosimetry.

4.5.5 Radiative Capture of Neutrons


When a neutron is absorbed by a nucleus any kinetic energy of the neutron plus its binding energy in the
resulting compound nucleus (usually 7 to 9 MeV) leaves the compound nucleus in a highly excited state.
The excited nucleus usually decays within 1 ps of the capture, often through several intermediate states,
thereby emitting one or more energetic gamma photons. These capture gamma photons from (n, γ) reactions
can be used to identify the isotope that absorbed the neutron.
126 Radiation Interactions in Matter Chap. 4

The cross section for radiative capture is very small for high energy neutrons, typically no more than
a few hundred millibarns for neutrons with energies between 20 keV and 10 MeV. For many nuclides, the
(n, γ) capture cross section is poorly known in the keV and MeV energy region. Only for certain important
nuclides such as fissionable isotopes is the cross section known with a good degree of certainty. Of more
importance are the (n, γ) reactions caused by thermal neutrons which have been slowed by scattering and
come into equilibrium with the thermal motion of atoms in the shield. The (n, γ) cross section for thermal
neutrons may be quite large—up to thousands of barns for nuclides such as cadmium that have capture
resonances near the thermal energy region—and for most isotopes it comprises almost the total absorption
cross section. In a material at room temperature, the thermal neutrons have an average energy of 0.025 eV,
corresponding to a speed of 2200 m s−1 . In Appendix B, thermal neutron cross sections, as well as yields
and energies of the capture photons, are given for common elements.

4.5.6 Neutron-Induced Fission


When a neutron is absorbed by a heavy nucleus, the resulting compound nucleus is produced in a very excited
state. The “nuclear fluid” of such an excited nucleus undergoes large oscillations and deformations in shape.
The compound nucleus may, during one of its oscillations in shape, deform into an elongated or dumbbell
configuration in which the two ends Coulombically repel each other and the nuclear forces, being very short
ranged, are no longer able to hold the two ends together. The two ends then separate (scission) within about
10−20 s into two nuclear pieces, repelling each other with such tremendous Coulombic force that many of
the orbital electrons are left behind. Two highly charged fission fragments are thus created.14 The fission
fragments are produced in such highly excited nuclear states that neutrons can “boil” off them. Anywhere
from 0 to about 8 prompt neutrons evaporate from the primary fission fragments within about 10−17 s of the
scission. After prompt neutron emission, the fission fragments are still in excited states, but with excitation
energies insufficient to cause further neutron emission. They quickly decay to lower energy levels only by
the emission of prompt gamma rays within about 2 × 10−14 s after the prompt-neutron emission.
The highly charged fission fragments pass through the surrounding medium producing millions of ioniza-
tions and excitations of the ambient atoms. As the fission fragments slow, they gradually acquire electrons
reducing their ionization charge, until, by the time they are stopped after about 10−12 s, they become electri-
cally neutral atoms. After prompt neutron and gamma ray emission, the fission fragments are then termed
fission products. The fission products are generally radioactive and, thus, start decay chains whose members
radioactively decay, usually by isobaric β − decay, until a stable end-nuclide is reached. Occasionally, short-
lived fission products decay by neutron emission producing delayed neutrons seconds to minutes after the
fission event. The half-lives of the many possible fission product daughters range from fractions of a second
to many thousands of years.
Sometimes very heavy radionuclides, e.g., 238 U and 252 Cf, are already sufficiently unstable that the
addition of a neutron is not needed to excite the nucleus to produce oscillations that lead to fission. Such
nuclides are said to spontaneously fission.

4.6 Charged-Particle Interactions


Knowledge of the ranges of ionizing charged particles and the rates at which energy is dissipated along their
paths is of crucial importance in the design of radiation detectors and in radiation dosimetry. A charged
particle is slowed as a result of both Coulombic interactions with (atomic) electrons and radiation losses
(bremsstrahlung). Energetic charged particles cause thousands of ionizations and excitations of the atoms
along their path before they are slowed and become part of the ambient medium.

14 Sometimes three fission fragments are formed in ternary fission with the third being a small nucleus. Alpha particles are
created in about 0.2% of the fissions, and nuclei of 2 H, 3 H, and others up to about 10 B are formed much less frequently.
Sec. 4.6. Charged-Particle Interactions 127

The stopping power, often denoted as −dE/dx, is the expected energy loss per unit distance of travel by
the charged particle along its trajectory. As used in this book, the term is synonymous with linear energy
transfer (LET), denoted as L(E). During deceleration, the stopping power generally increases until the
energy of the particle is so low that charge neutralization or quantum effects bring about a reduction in the
rate of energy loss.
Unlike photons and neutrons, charged particles have a finite range in matter, i.e., there is a distance
beyond which none can travel. The distance the particle travels before being stopped is called the range.
However, this definition is not very precise because, for stochastic reasons, not every particle starting with
the same energy travels the same distance before stopping. Also the distance used to define the range can be
either along the particle’s trajectory or a straight-line (crow-flight) distance from the source of the charged
particles. The resulting slightly different definitions of range are described more fully later in this section. A
charged particle range is often reported as a mass thickness range defined as R/ρ, with units such as g cm−2 ,
in order to mostly remove the density dependence of the range on the density ρ of stopping medium. The
paths traveled by light particles, like electrons and positrons, are quite different from those of heavy charged
particles such as protons and alpha particles, and are considered separately in the following sections.
Heavy charged particles (HCPs) are ions with masses greater than or equal to that of a proton. With
kinetic energies much less than their rest-mass energies, HCPs lose energy almost entirely from Coulombic
interactions with atomic electrons. A multitude of such interactions take place—so many that the slowing
down is virtually continuous along a straight-line path. These interactions, taken individually, may range
from ionization processes producing energetic recoil electrons called delta rays to weak atomic or molecular
excitation, which may not result in ionization at all. The LET resulting from Coulombic interactions, Lcoll ,
is called the collisional LET or collisional stopping power. Only for heavy charged particles of very low
energy do collisions with atomic nuclei of the stopping medium become important and can result in large
angular deflections from their usual straight-line trajectories.
Another energy-loss mechanism, which is especially important for electrons, is radiative energy loss
through bremsstrahlung production and is characterized by the radiative LET or radiative stopping power
Lrad . Also, a careful treatment of electron slowing down requires consideration of delta-ray production and
the concomitant deflection of the incident electron from its original direction. As a result the trajectory of
slowing electrons is tortuous exhibiting many large angle deflections.
The total stopping power is defined as
 
dE dE  dE 
L=− =− − , (4.111)
dx dx coll dx rad
which is the sum of the collisional and radiative energy losses. The mass stopping power is defined as
L dE 1
=− , (4.112)
ρ dx ρ
where ρ is the mass density of the stopping material, and has units such as MeV cm2 g−1 . Also, the specific
ionization is defined as
L dE 1
=− , (4.113)
w dx w
where w is the average energy required to liberate an electron from its host atom, usually described as the
production of electron-ion pairs (gases) or electron-hole pairs (solids).

4.6.1 Collisional Energy Loss


Collisional energy loss results from momentum transfer caused by the Coulombic force between the incident
particle with speed v and charge number z and the target, of mass M , which is an atomic nucleus with
128 Radiation Interactions in Matter Chap. 4

charge number Z equal to the atomic number, or an electron of charge number Z = 1. The kinematics of
individual interactions were described earlier in this chapter with notation as illustrated in Fig. 4.2. The
LET may be computed on the basis of a differential interaction cross section dσ(E, T )/dT defined so that
[dσ(E, T )/dT ] dT is the cross section for interaction of an incident particle of energy E, resulting in a target
recoil with energy between T and T + dT . A differential linear interaction coefficient dμ(E, T )/dT is the
product of dσ(E, T )/dT and the density N of targets, atomic nuclei, or atomic electrons, as appropriate.
The product T [dμ(E, T )/dT ] dT is the total energy loss per unit differential distance of travel of the primary
particle associated with individual losses between T and T + dT . Thus, the LET L(E) is given, in principle,
by
 Tmax
dμ(E, T )
L(E) = T dT. (4.114)
0 dT
The total LET is the sum of the collisional and radiative LETs, Lcoll (E) + Lrad (E) based on integrals over
dμcoll (E, T )/dT and dμrad (E, T )/dT .
Rutherford Cross Section
The fundamental formula for collisional loss, named for Ernest Rutherford (1871–1937), is based on classical
mechanics and was originally derived for scattering of alpha particles by atomic nuclei. Its derivation may
be found in most textbooks on atomic and nuclear physics. A rigorous derivation, based on conservation
of angular momentum as well as kinetic energy and linear momentum, may be found in Evans [1955]. The
differential cross section may be written as
σruth (E, T ) 2πz 2 Z 2 qe4 2πz 2 Z 2 qe4 1
= 2 2 2
= , (4.115)
dT (4πo ) M v T (4πo ) M c β T 2
2 2 2

in which qe is the unit electronic charge. Note that if targets are atomic electrons, their density is Ne =
ρ(Z/A)Na , where Z is the medium atomic number. Then M = me and the target charge number is unity.
In terms of dimensionless variables  = E/me c2 and τ = T /me c2 , and with dμ(, τ )/dτ = me c2 dμ(E, T )/dT ,
the linear coefficient for interactions with atomic electrons is given by
dμruth (, τ ) 2πNe z 2 re2 1
= , (4.116)
dτ β2 τ2
in which re is the classical electron radius, given in Eq. (4.62). Equation (4.115) commonly appears in the
cgs system of units, within which the factor 4πo does not appear and re = qe2 /me c2 . Bhabha [1938] showed
that for heavy charged incident particles and electron targets, the Rutherford cross section must be modified
to
dμcoll (, τ ) 2πNe z 2 re2 1 β2
= 2 2
− , (4.117)
dτ β τ τ τmax
where τmax ≡ Tmax /me c2 , with Tmax being the maximum energy transferred to the recoil particle (see
Section 4.3.8). This equation applies to alpha particles or other particles with spin 0. An additional
correction term, important only for highly relativistic conditions, is required for protons or particles with
spin 1/2.
Møller and Bhabha Cross Sections
The relativistic collisional energy loss in electron-electron interactions was addressed by Møller [1932], who
found that
dμcoll (, τ ) 2π Ne re2 1 1 1 2 + 1
= + + − . (4.118)
dτ β 2 τ 2 ( − τ )2 ( + 1)2 τ ( − τ )( + 1)2
This interaction coefficient is illustrated in Fig. 4.17. A similar expression for positron energy losses was
derived by Bhabha [1936].
Sec. 4.6. Charged-Particle Interactions 129

"

!

)
r A 
A
N ε = 0.5
π

2(
/) 
, ε = 1.0
ε τ

( ll
o ε = 2.0
k
c

ε = E/m A c
ε = 5.0
-  τ = T/ m A c
ε = 10

-
-   

τ
Figure 4.17. Møller cross section for electron-electron interactions.

Collisional LET
Both the classical and the relativistic approaches fail when Eq. (4.116) or (4.118) is substituted into
Eq. (4.114). The integral dτ τ −2 is infinite for a lower limit of zero. However, the zero limit is not
realistic physically. A quantum mechanical approach is necessary because energy losses less than some finite
value are prohibited due to quantized states of atomic electrons in the stopping medium. Bethe [1930, 1932]
showed that the collisional LET can be written in the form
 τmax
1 ρZz 2 C
Lcoll () = 2πz 2 Ne me c2 re2 2 dτ τ [τ −2 + · · ·]  ¯
f (τmax , I), (4.119)
β 0 Aβ 2

in which C = 4πNa re2 me c2 = 0.30705 cm2 MeV mol−1 . In the function f , I¯ ≡ I/me c2 is a dimensionless
mean excitation energy and is determined empirically for the stopping medium. Note that when the target
is an electron ⎧
⎨ /2 for electron collisions,
τmax =  for positron collisions, (4.120)

2β 2 /(1 − β 2 ) for non-relativistic heavy particles.

Selected values of I are given in Table 4.2. For Z ≥ 13, I for elemental substances, in units of eV, is
given approximately by the empirical formula [Barkas and Berger 1964]

I = 9.76Z + 58.8Z −0.19. (4.121)

Janni [1982] gives the following formula, valid within 10% for Z > 34:

I = 10.3Z − 8.17Z 1/3. (4.122)


130 Radiation Interactions in Matter Chap. 4

Table 4.2. Selected values of the mean excitation energy for compounds and atomic
constituents of compounds in the condensed state.
Material Form I (eV) Material Form I (eV)
H saturated bond 19.0 H2 gas 19.2
H unsaturated bond 16.0 N2 gas 82.0
C saturated bond 81.1 O2 gas 95.0
C unsaturated bond 79.8 CO2 gas 85.0
C highly chlorinated 69.0 Air dry 85.7
N amines, nitrates, etc. 105.7 Water gas 71.6
N in rings 81.9 Water liquid 75.0
O –O– 104.6 Tissue ICRU muscle 74.7
O =O 94.4 Bone ICRU compact 91.9

Source: ICRU [1984].

For atomic constituents of compounds, I should be increased by a factor of 1.13 [ICRU 1984]. For mixtures
of elements identified by the index j, the average values of Z/A and I are given by the empirical formulas
  Zj 
Z/A = wj (4.123)
j
Aj

and  
 Zj
−1
ln I = Z/A wj ln Ij . (4.124)
j
Aj

in which wj is the weight fraction of the jth constituent.

4.6.2 Radiative Energy Loss


Classical electromagnetic theory requires that the rate at which electromagnetic energy is radiated from
an accelerating charged particle be proportional to the square of the acceleration. In the electric field of a
nucleus with atomic number Z, the force on a charged particle with z elemental charges is proportional to
the product Zz. The resulting acceleration of the charged particle is proportional to this force and inversely
proportional to the particle’s mass m. Thus, the rate of radiative energy loss by the charged particle would
be expected to be proportional to (Zz/m)2 . This inverse-square dependence on particle mass explains why
bremsstrahlung from protons or heavier charged particles is negligible in most circumstances compared to
that from electrons or positrons. The dependence on the square of Z also explains why, except for the
lightest elements, bremsstrahlung in the field of the nucleus far exceeds bremsstrahlung in the fields of
atomic electrons.
One may define a differential interaction coefficient for radiative energy loss in such a way that
μrad (E, E  ) dE  is the probability per unit differential distance of travel that deceleration of an electron
of energy E results in emission of a photon with energy between E  and E  + dE  . However, it is not possible
to write a simple expression for μrad (E, E  ) or for the associated microscopic cross section σrad (E, E  ). The
interaction coefficient for radiative energy loss by an electron is illustrated in Fig. 4.18, which is based on
calculations performed by the PEGS4 computer program [Nelson et al. 1985].
For a relativistic heavy charged particle of rest mass M , with E M c2 , it can be shown that the ratio
of radiative to ionization losses is approximately [Evans 1955]

(−dE/ds)rad EZ me 2
 , (4.125)
(−dE/ds)coll 700 M
Sec. 4.6. Charged-Particle Interactions 131

1.

 0.8
 
 2 MeV

 0.6 5 MeV


 
')
E,
(E 0.4
@
H=
μ

E
0.2

0.0
- -  


Figure 4.18. Energy spectrum of bremsstrahlung photons released


in lead by radiative energy losses of electrons with initial energy E.

where E is in MeV. From this result it is seen that bremsstrahlung is more important for high-energy particles
of small mass incident on high-Z material. In most dosimetry situations, only electrons (me /M = 1) are of
importance for their associated bremsstrahlung. All other charged particles are far too massive to produce
significant amounts of bremsstrahlung. Bremsstrahlung from electrons is of particular radiological interest for
devices that accelerate electrons, such as betatrons and x-ray tubes, or for situations involving radionuclides
that emit only beta particles.

4.6.3 Estimating Charged-Particle Ranges


Charged particles as they travel through some medium lose energy through Coulombic interactions with am-
bient electrons (and, infrequently, with atomic nuclei) and by bremsstrahlung production. As a consequence,
they eventually come to rest (discounting thermal motion) after a finite distance of travel. The distance a
charged particle travels before coming to rest is called its range. However, there are several measures used
for the range of a charged particle.
The Continuous Slowing Down Range
It is common to neglect energy-loss fluctuations and assume that particles lose energy continuously along
their tracks, with a mean energy loss per unit path length given by the total stopping power. Under this
approximation [ICRU 1984], the continuous slowing down range RCSDA of a charged particle with initial
kinetic energy Eo is given by [ICRU 1984]
 R  Eo
dE
RCSDA = ds = . (4.126)
0 0 (−dE/ds) tot

where (−dE/ds)tot = (−dE/ds)coll + (−dE/ds)rad , the total stopping power. This range is the expected
length of a particle’s trajectory before it comes to rest.
Evaluation of the integral is complicated by difficulties in formulating both the radiative stopping power
and the collisional stopping power for low-energy particles, particularly electrons, and it is common to assume
that the reciprocal of the stopping power is zero at zero energy and increases linearly to the known value
at the least energy. It should be noted that this range cannot be measured experimentally since, to do so,
would require a three-dimensional visualization of a particle’s track and an evaluation of the length of this
track.
132 Radiation Interactions in Matter Chap. 4

Ranges for Penetration Depths


For a charged particle of a specific type traveling in a given medium, there is some average distance the
particle travels between where it starts with energy E0 and where it comes to rest and becomes part of the
ambient medium. The mean forward or projected range Rp is the expected or average maximum depth of
penetration in the initial direction of the charged particle. This range can be measured experimentally by
finding the distance from a monodirectional source along the emission direction at which the intensity of
charged particles is reduced by 50%.
Because charged particles, especially electrons and positrons, can be backscattered as they slow down,
another range, which is sometimes encountered, is the average penetration distance Rend to where the particle
comes to rest, i.e., to where the particle trajectory ends. As in the definition of Rp , this range is defined
along a straight line in the initial particle direction. For HCPs Rp ≤ Rend but for electrons Rend can be
substantially smaller than Rm .
There are other ranges that are sometimes encountered for heavy charged particles. One is the maximum
range Rmax that is the crow-flight distance, in the initial particle direction, between the particle source to
a point beyond which no particle reaches. Yet another straight-line range is the extrapolated range Re that
is based on a linear extrapolation of the distance versus intensity plot from Rp to zero intensity. These two
ranges are discussed in more detail later in this section.
The CSDA and projected ranges are non-stochastic quantities and for heavy charged particles are nearly
equal. For electrons, however, RCSDA can be significantly greater than Rp and Rend . This difference is
quantified by the detour factor, discussed next.
Detour Factor
The difference between RCSDA and Rp is due to the deviation of a charged particle’s trajectory from an
ideal straight-line trajectory, a result of the multiple scattering events that occur along the trajectory. This
deviation is very pronounced for electrons and positrons but much less so for heavy charged particles. The
detour factor is defined as Rp /RCSDA [Andreo et al. 2017]. It should be noted that this definition is subtly
different for protons and alpha particles as defined by the ICRU [1993] who, instead of Rp used Rend , the
depth of penetration to the termination point. Examples of the detour factor for electrons, protons and
alpha particles are shown in Fig. 4.19 where it is seen that electrons have smaller detour factors than the
heavy charged particles. This difference is a consequence of the much more tortuous path an electron travels
while traversing matter compared to the path taken by a heavy charged particle.

4.6.4 Electron Energy Loss and Range


Before modern-day computers, analytical expressions were used to approximate the energy loss of electrons
through matter. One widely used expression for relativistic electrons, based on the electron scattering results
of Møller [1932], was derived by Bethe for electron stopping power in a substance with electron density Ne
[Bethe and Ashkin 1953]
" 
2πNe qe4 mv 2 E
L= ln − 2 1 − β 2 − 1 + β 2 ln 2
mv 2 2I (1 − β)
2

 #
1
+1 − β 2 + (1 − 1 − β 2 )2 . (4.127)
8

where E is the incident particle energy and I is the average excitation potential. Although generally conve-
nient for a wide variety of materials, Eq. (4.127) becomes inaccurate at low electron velocities. More recently,
computer codes with corrections to the Bethe equation render improved results. For electrons and positrons,
integration of the Møller [1932] or Bhabha [1938] cross section, with z = 1, leads to the Rohrlich and Carlson
Sec. 4.6. Charged-Particle Interactions 133

Figure 4.19. Detour factors Rp /RCSDA for electrons (heavy dashed


lines), protons (solid lines) and alpha particles (light dashed lines).
The data for protons and alpha particles were obtained with the
STAR codes [Berger 1992] and for electrons from Andreo et al. [2017].

[1954] formula used by Seltzer and Berger [1985; 1986] in their compilations of stopping powers [ICRU 1984]
ρZC  
¯ + ln(1 + /2) + F ± () − δ .
Lcoll (E) = 2
2 ln(/I) (4.128)
2Aβ

The factor F − for electrons is given by


 
F − () = (1 − β 2 ) 1 + 2 /8 − (1 + 2) ln 2 . (4.129)

The factor F + for positrons is given by


 
F + () = 2 ln 2 − (β 2 /12) 23 + 14/( + 2) + 10/( + 2)2 + 4/( + 2)3 . (4.130)

In Eq. (4.128), the density-effect correction term δ accounts for polarization of atoms in the stopping medium
caused by passage of the electron, the result of which is a reduction of the electric field acting on the moving
electron and thus a reduction in the stopping power. Evaluation of δ is quite involved. Procedures are
described by the ICRU [1984]. In liquid water, for example, the density effect causes a 1.2% reduction in
Lcoll at E = 1 MeV, 3.9% at 2 MeV, and 11.5% at 10 MeV. Selected values of mean excitation energies are
given in Table 4.2. Stopping powers are illustrated in Fig. 4.20.
Restricted Electron Stopping Power The rate at which energy is deposited locally along the track of an
electron is of great importance in certain radiation detector analyses. This requires establishing a cutoff
energy, say Ecut , below which an energy loss is considered to be local. A value of Ecut on the order of 200
134 Radiation Interactions in Matter Chap. 4

Figure 4.20. Linear energy transfer L/ρ in mass units (MeV cm2 /g) for alpha particles,
protons and electrons. The dashed line for aluminum is the collisional LET for positrons.
Data is from the STAR series of codes [Berger 1992].

eV is often chosen. The restricted stopping power Lcoll (E, Ecut ) is defined in analogy with Eq. (4.119), but
with τmax expressed in terms of Ecut . The result is

ρZC  
¯ + ln(1 + /2) + G± (, η) − δ ,
Lcoll (E, Ecut ) = 2
2 ln(/I) (4.131)
2Aβ

in which η ≡ Ecut /E. The factor G− for electrons is given by


 
G− (, η) = (1 − β 2 ) 2 η 2 /2 + (2 + 1) ln(1 − η) − 1 − β 2 + ln [4η(1 − η)] + (1 − η)−1 . (4.132)

The factor G+ for positrons is given by

G+ (, η) = ln 4η − β 2 [1 + (2 − ξ 2 )η − (3 + ξ 2 )(ξ/2)η 2
+ (1 + ξ)(ξ 2 2 /3)η 3 − (ξ 3 3 /4)η 4 ], (4.133)

in which ξ ≡ ( + 2)−1 .
Electron Radiative LET No simple formula can describe the stopping power or LET for electron radiative
energy losses (bremsstrahlung). The total stopping power can be written as the sum of stopping powers
associated with radiative losses in the force fields of nuclei and electrons, namely, Lrad (E) = Lrad,n(E) +
Lrad,e (E) = Lrad,n (E)(1 + ξ/z), in which ξ is the “correction term” Lrad,e /Lrad,n. According to ICRU
[1984], ξ depends hardly at all on the medium and is less than 1.2 in magnitude for all E. It is about 0.5 at
E = 700 keV and approaches zero at low E. The radiative stopping power may be written as [ICRU 1984]

Lrad (E) = N re2 (E + me c2 )Z 2 α(1 + ξ/Z)Φ(E, Z), (4.134)


Sec. 4.6. Charged-Particle Interactions 135

Z=1


)
Z,
E 
( $
@
H=
!
Φ

$
 %'

 -
 -     


Figure 4.21. Scaled dimensionless radiative energy loss cross sections


Φrad (E, Z) for electrons in various media. Based on data from Seltzer and
Berger [1986].

in which N is the atomic density, α  1/137 is the fine-structure constant, and Φ(E, Z) is the dimensionless
scaled radiative energy-loss cross section given by
 E
1
Φ(E, Z) = dE  E  σrad (E, E  ). (4.135)
αre2 Z 2 (E + me c2 ) 0
The function Φ, too, is not strongly dependent on Z, as is illustrated in Fig. 4.21 for several values of Z.
Tables of data are given by Seltzer and Berger [1985, 1986].
Electron Range The mean crow-flight range of electrons in a material with density ρ can be approximated
by [Katz and Penfold 1952]
$
0.412E 1.265−0.0954 ln E 0.1 MeV ≤ E ≤ 3 MeV
−2
ρRp (g cm ) = , (4.136)
.530E − 0.106 2.5 MeV ≤ E ≤ 20 MeV
where E is the energy of the incident electron. Notice that this empirical approximation is independent of
the Z number of the attenuating material, a result that follows from the observation that, when the range
is expressed in terms of mass thickness, the range is almost the same for all materials (as can be seen from
Fig. 4.23).
When determining the maximum range of beta particles, then the maximum particle emission energy
should be used. Notably, Eq. (4.136) implies that the electron mass range ρRp is independent of the target
material. The usefulness of this outcome allows easy range estimations between differing materials. Hence,
the result of Eq. (4.136) need only be divided by the mass density of the target material to determine the
actual range. However, in reality there is a difference in particle range between materials, and modern
computer programs can provide better range estimates than the older empirical formulas.
Beta particles (electrons or positrons) produce numerous ionizations and electronic excitations as they
move through a medium. Most interactions are small deflections accompanied by small energy losses. How-
ever, beta particles, having the same mass as the electrons of the medium, can also undergo large-angle
136 Radiation Interactions in Matter Chap. 4

Figure 4.22. Tracks of 30 electrons from a 50-keV (left) and a 1-MeV (right) point isotropic source
in water, shown as orthographic projections of tracks into a single plane. The box has dimensions
2ro × 2ro where ro is the CSDA range of the electrons. Calculations performed using the EGS4 code,
courtesy of Robert Stewart, Kansas State University.

scatters producing secondary electrons with substantial recoil energy. These energetic secondary electrons
(called delta rays) in turn pass through the medium causing additional ionization and excitation. Large-angle
deflections from atomic nuclei can also occur with negligible energy loss. Consequently, the paths traveled
by beta particles as they transfer their energy to the surrounding medium are far from straight. Examples
of such paths are shown in Fig. 4.22.
For such paths, it is seen that the distances beta particles travel into a medium vary tremendously. The
range of beta particles is defined as the path length of the particles, i.e., the distance they travel along their
twisted trajectories. This range is well approximated by the CSDA range and is the maximum distance a
beta particle can penetrate, although most, because of the twisting of their paths, seldom penetrate this far
(see Section 4.6.3).
It may be inferred from data given by Cross, Freedman, and Wong [1992] that for a beam of electrons,
ranging in energy from 0.025 to 4 MeV, normally incident on water, about 80% of the electron energy is
deposited within a depth of about 60% of the CSDA range, 90% of the energy within about 70% of the
range, and 95% of the energy within about 80% of the range. For a point isotropic source of monoenergetic
electrons of the same energies in water, 90% of the energy is deposited within about 80% of the range, and
95% of the energy within about 85% of the range. In either geometry, all of the energy is deposited within
about 110% of the CSDA range. Electron CSDA ranges are presented in Fig. 4.23.

4.6.5 Spatial Distribution of the Electron Energy Absorption


In both the design of radiation detectors and radiation dosimetry, it is important to know where the energy
of a charged particle is deposited at different distances from the source of the charged particles. Because of
the tortuous trajectories of electrons, the spatial distribution of this absorbed energy is not easily calculated
from first principles. This section considers point and uniform-beam sources of monoenergetic electrons
in infinite homogeneous media. In particular, spatial distributions of the absorbed dose (absorbed energy
per unit mass) are expressed in terms of point and plane kernels and associated scaled dimensionless dose
distributions.
Sec. 4.6. Charged-Particle Interactions 137

Figure 4.23. The CSDA range or path length ρR, in mass thickness (g/cm2 ),
for electrons in various materials. The CSDA ranges are shown as solid black
lines. Also shown, as gray dotted lines, are linear energy transfer (LET) as
functions of energy. Data are from the STAR series of codes [Berger 1992].

Point and Plane Kernels Defined


The expected absorbed dose at distance r from a unit point isotropic source of monoenergetic charged
particles of energy E is denoted as G(r, E). Typical units for G are MeV/g. The point kernel G is very
conveniently expressed in terms of the dimensionless dose distribution F (r/ro , E), with radial distance r
scaled by the CSDA range RCSDA ≡ ro , namely,

E E
G(r, E) = F (r/ro , E) = F (r̂/r̂o , E), (4.137)
4πr2 ρro 4πr2 r̂o

in which r̂ = ρr and r̂o is the CSDA range of Eq. (4.126) in mass units. A useful interpretation of F , which
is illustrated in Fig. 4.24, is that the fraction of E deposited between radii r and r + dr is (dr/ro )F (r/ro , E).
Note that, without a subscript, F and G refer to a point isotropic source.
Similarly, for an infinite plane perpendicular15 source of monoenergetic particles in an infinite homoge-

neous medium, the expected absorbed dose at distance r along the beam is denoted as Gpl (r, E). This is
conveniently expressed in terms of a scaled dimensionless dose distribution as

⊥ E ⊥
Gpl (r, E) = F (r/ro , E), (4.138)
ρro pl

which is illustrated in Fig. 4.25.

15 The source is an area source with all particles released in a parallel beam normal to the source area.
138 Radiation Interactions in Matter Chap. 4

Figure 4.24. Scaled dimensionless dose dis- Figure 4.25. Comparison of F (r/ro , E)
tributions, F (r/ro , E), for point isotropic point-source, Fpl ⊥ (r/r , E) parallel-beam-
o
electron sources in water. From Cross, source, and CSDA scaled dimensionless dose
Freedman, and Wong [1992]. distributions for 2-MeV electron sources in
water. Data for the point and parallel-beam
sources from Cross, Freedman, and Wong
[1992].

CSDA Absorbed Energy Distribution


In the continuous slowing-down approximation, all particle tracks are straight and of length ro . It is easily
shown that in this approximation,
 ⊥  L(ro − r)
Fpl (r, E) CSDA = [F (r, E)]CSDA = , r < ro . (4.139)
E/ro
Note that the linear energy transfer L is evaluated at the energy of the particle after passage through distance
r, that is, for a particle with residual range ro − r. The residual range16 determines both the energy and
the LET of a particle. The denominator of Eq. (4.126) is just the average LET along the entire path of the
particle. Point and plane dose distributions are compared with the distribution in the CSDA approximation
in Fig. 4.25.
Electron Absorbed Energy Distributions
The pioneering moments-method electron-transport calculations of Spencer [1959] were used by Berger [1971]
and Cross et al. [1982] to construct scaled dimensionless dose distributions for monoenergetic electrons and
beta-particle sources. These were revised by Berger in 1973, based on Monte Carlo calculations. Cross,
Freedman, and Wong [1992] also used Monte Carlo methods to prepare comprehensive tables of dose dis-
tributions for point, plane parallel, and plane isotropic sources of electrons and beta particles in water.
Example dose distributions for point sources are illustrated in Fig. 4.25. Tabulations of F (r/ro , E) versus
r/ro are given by Shultis and Faw [2000] and Cross et al. [1992].
Figure 4.25 compares kernels for 2-MeV point and plane parallel electron sources in water. In contrast, the
point kernel based on the CSDA approximation is shown to be a very poor approximation for electrons. The
reason is apparent from examination of Fig. 4.22, which shows the spatial distributions of energy deposition
from point isotropic sources of monoenergetic electrons. Not only is much of the energy deposited well within

16 Acharged particle energetic enough to penetrate a distance x and emerge with energy E  has a residual range RCSDA (E  ) in
the same material. So the range RCSDA (E) of the particle with initial energy E must have been x + RCSDA (E  ).
Sec. 4.6. Charged-Particle Interactions 139

distance ro , but the spatial distribution of the energy distribution scaled by ro is insensitive to E. The scaled
patterns shown in Fig. 4.22 for 50-keV and 1-MeV electrons reinforce the logic for the similarity in shapes
of the curves in Fig. 4.24.
Kernels in Non-Aqueous Media
It has long been observed [Cross 1967; Berger 1971] that when distance is measured in mass thickness r̂ = ρr,
the point kernel in medium m at distance r̂ is proportional to that in water, medium w, at a scaled distance
ηr̂. The scale factor η was found to depend on medium m but only very weakly on the energy, so that
the same scale factor could be applied to beta-particle sources as well as monoenergetic electron sources.
Conservation of energy for a point source requires that
 ∞  ∞
d(r̂/ρm ) (r̂/ρm )2 ρm Gm (r̂, E) = d(ηr̂/ρw ) (ηr̂/ρw )2 ρw Gw (ηr̂, E). (4.140)
0 0

It therefore follows that


2
ρm
Gm (r̂, E) = η 3 Gw (ηr̂, E). (4.141)
ρw
Similarly,
⊥ ⊥
Gm,pl (r̂, E) = η Gw,pl (ηr̂, E). (4.142)
In terms of the dimensional dose distribution F the point kernel for medium m is
   
E r̂ E r̂
Gm (r̂, E) = F ,E = F ,E , (4.143)
4πr2 (r̂o /η) r̂o /η 4πr2 r̂m r̂m

in which the mass CSDA range r̂m (E) of electrons in medium m, in terms of that in water, is given by
r̂m (E) = r̂o (E)/η. Thus, F may be interpreted as a universal function of the ratio r̂/r̂m = r/rm , the
distance from the point source in units of the CSDA range.
Cross, Freedman, and Wong [1992] recommend that η be computed using the following formula, which
is based on experiments and calculations for beta-particle attenuation in various media relative to that in
water:
2 (L/ρ)m
η = 0.77(1 + 0.0491Z − 0.0009Z ) , (4.144)
(L/ρ)w
in which the mean atomic number is given as follows, based on mass fractions of the atomic constituents in
the medium: %
wi Zi2 /Ai
Z = %i . (4.145)
i wi Zi /Ai

The ratio of stopping powers is insensitive to energy, and Berger [1971] recommends that they be evaluated
at 0.2 MeV. Cross, Freedman, and Wong [1992] recommend that, instead, (L/ρ)m /(L/ρ)w be replaced by
r̂w /r̂m evaluated at 500 keV. These formulas predict that η = 0.89 for air. Note that the ratio of the mass
CSDA range in water to that in air varies from 0.89 for 0.01-MeV electrons to 0.91 for 3-MeV electrons. For
the human body, η is 0.98 for soft tissue and 0.97 for compact bone.

4.6.6 Heavy Charged-Particle Energy Loss


Rossi [1952] describes the stopping power for relativistic heavy charged particles as
 
ρZz 2 C 2β 2
Lcoll (E) = ln − β2 . (4.146)
Aβ 2 (1 − β 2 )I¯
140 Radiation Interactions in Matter Chap. 4

This approximation is mainly used for protons with energies between about 10 and 1000 MeV or other heavy
particles with comparable speeds. Note that Lcoll is directly proportional to z 2 and that Ne = ρ(Z/A)Na .
It does not vary independently with mass and kinetic energy of the incident charged particle. Instead, Lcoll
is a function of the particle velocity or β 2 .
At low energies, β becomes small and Eq. (4.146) reduces to
 
ρZz 2 C 2me v 2
Lcoll (E) = ln . (4.147)
Aβ 2 I

Note that Lcoll is only weakly dependent on the mean excitation energy I. For a non-relativistic particle,17
v = 2T /M . Thus, in a given medium, a 1-MeV proton has roughly the same collisional stopping power
as a 2-MeV deuteron and roughly one-fourth that of a 4-MeV alpha particle. In this way, stopping-power
data for protons may be used to approximate stopping powers for other heavy charged particles. Equation
(4.146) overestimates the LET by less than about 10% for proton energies between 1 and 104 MeV and for
stopping media such as air, water, and elements ranging in atomic number from aluminum to gold. For
proton energies much below 1 MeV, the formula fails utterly. For low energies, Anderson and Ziegler [1977]
recommend a general relation
Lcoll (E)  A1 E A2 , (4.148)
where A1 is an experimentally determined constant and A2  0.5. The collisional stopping power for protons
and alpha particles, as a function of the particle’s energy, is shown in Fig. 4.20.
Corrections to Eq. (4.146) account for shell and density effects, among other minor effects. Shell correc-
tions compensate for the fact that the atomic binding of inner-shell electrons reduces their participation in
charged-particle slowing down. Density corrections compensate for the polarization of the stopping medium
induced by passage of the charged particle and the resulting perturbation of the electronic structure and
reduction in stopping power. Stopping of low-energy charged particles is affected by neutralization of the
charge of the particle and by collisions with atomic nuclei of the stopping medium. Detailed data on the
LET and range of heavy charged particles are given in reports by Janni [1982], Hubert et al. [1990], and
the ICRU [1993]. Computer codes are also available for calculation of ranges, stopping powers, and related
quantities for electrons, protons, helium nuclei, and heavy ions [Berger 1992; Ziegler et al. 2013].

4.6.7 Heavy Charged-Particle Range


When a heavy charged particle (HCP) with mass M and energy EM scatters from an electron, the maximum
energy loss by the HCP and the maximum energy of the recoil electron is [Shultis and Faw 2017]
me
(Ee )max = 4 EM . (4.149)
M
As an example, consider a 4-MeV alpha particle. From Eq. (4.149), the maximum energy loss of such an
alpha particle when it interacts with an electron is found to be 2.2 keV. Most such alpha-electron interactions
result in far smaller energy losses, although usually sufficient energy transfer to free the electron from its atom
or at least to raise the atom to a high excitation state. Consequently, many thousands of these interactions
are required for the alpha particle to lose its kinetic energy.
Moreover, the mass of the alpha particle being over 7000 times that of an electron, the alpha particle
experiences negligible deflection from its path of travel. An important characteristic of such heavy charged
particles, as they move through a medium, is that they travel in almost straight lines, unless they are

17 By
this is meant a particle whose kinetic energy is very much less than its rest-mass energy: 511 keV for electrons, about 930
MeV for protons or neutrons, and about 3727 MeV for alpha particles.
Sec. 4.6. Charged-Particle Interactions 141

Figure 4.26. Fraction of α-particles that penetrate a distance s.


The gray dotted line shows the derivative dn(s)/ds and is termed the
straggling curve, a result of the large-angle scattering near the end
of the particles’ paths and the statistical fluctuations in the number
of interactions needed to absorb the particles’ initial energy.

deflected by a nucleus. Such nucleus-particle interactions are rare and usually occur only when the charged
particles have lost most of their kinetic energy.
Many measurements of the range of heavy particles have been made. In Fig. 4.26, the fraction of alpha
particles, with the same initial energy, that travel various distances s into a medium is illustrated. We see
from this figure, that the number of alpha particles penetrating a distance s into a medium remains constant
until near the end of their range. The number penetrating beyond this maximum distance falls rapidly.
The distance a heavy charged particle travels in a medium before it is stopped is not a precise quantity
because of the stochastic nature of the number and energy losses of all the particle-medium interactions,
and because of possible large-angle deflections near the end of the path. From Fig. 4.26, we see that the
range of a heavy charged particle is not an exact quantity. Several measures of the range can be defined. We
can define Rp as the mean or projected range, that is, the distance at which the intensity of heavy particles
has been halved. This projected range is at the maximum of the differential energy curve or straggling
curve dn(s)/ds, shown as the dotted curve in Fig. 4.26. Alternatively, the range can be taken as Re , the
extrapolated range, that is, the value obtained by drawing the tangent to the curve at its inflection point
and extrapolating the tangent until it crosses the s-axis. Finally, if we treat the slowing down of heavy
charged particles as a continuous process, a unique range, called the continuous slowing-down approximation
(CSDA), a unique CSDA range can be calculated. Although slightly different, all three of these definitions
of a heavy particle’s range are, for practical purposes, nearly the same. The mean and CSDA ranges for
protons and alpha particles are presented in Fig. 4.27.
Because of the large number of interactions with electrons of the ambient medium, heavy charged particles,
of the same mass and initial kinetic energy, travel in straight lines and penetrate almost the same distance
into a medium before they are stopped. Because of the stochastic nature of the particle-medium interactions
and because, near the end of their paths, some heavy particles experience large angle deflections from atomic
nuclei, the penetration distances exhibit a small variation called straggling. The straggling is defined by a
range-straggling parameter α0 , where α0  0.015Rp [Evans 1955]. The straggling curve indicates the final
142

Figure 4.27. Range or path length ρR, in mass thickness (g/cm2 ), for protons and alpha particles in several materials. The average (or projected)
ranges are shown as black solid lines while the CSDA ranges are shown as gray dotted lines. Data are from the STAR series of codes [Berger 1992].
Radiation Interactions in Matter
Chap. 4
Sec. 4.6. Charged-Particle Interactions 143

resting distribution of ions in the target material, and is modeled as a Gaussian distribution

1 dn(s) 1 2
= √ e−[(s−Rp )/α] , (4.150)
n0 ds α π

where n0 is the total number of ions and α  2α0 . Notably, the width 2α marks the locations in the
number-range curve where the maximum of Eq. (4.150) is reduced by e−1 .
For heavy charged particles, we may use Eq. (4.126) to obtain the dependence of the range on the particle’s
mass m and charge z. Because bremsstrahlung is seldom important for heavy charged particles with energies
below several tens of MeV, we may take (−dE/ds)tot  (−dE/ds)coll . From Eq. (4.146) we see the collisional
stopping power is of the form (−dE/ds)coll = ρ(Z/A)z 2 f (v) where f (v) is a function only of v or β = v/c.
From Eq. (4.126), the mass thickness range, ρRCSDA is
 Eo  Eo
dE 1 dE
ρRCSDA = ρ =ρ dv. (4.151)
0 (−dE/ds)coll 0 (−dE/ds)coll dv

Substitution of dE/dv = mv and (−dE/ds)coll = ρ(Z/A)z 2 f (v) then gives


    
A m vo v dv A m
ρRCSDA = 2
= g(vo ), (4.152)
Z z 0 f (v) Z z2

where g(vo ) is a function only of the initial speed vo of the particle. From this result, three useful “rules”
for relating different ranges follow.

1. The mass-thickness range ρRCSDA is independent of the density of the medium.


2. For particles of the same initial speed in the same medium, ρRCSDA is approximately proportional to
m/z 2, where m and z are for the charged particle.

3. For particles of the same initial speed, in different media, ρR is approximately proportional to
(m/z 2 )(Z/A), where Z is the atomic number of the stopping medium and A is its atomic weight.

Thus, from rule 2, in a given medium, a 4-MeV alpha particle has about the same range as a 1-MeV
proton. However, these rules fail for particle energies less than about 1 MeV per atomic mass unit. For
example, the CSDA range of a 0.4-MeV alpha particle in aluminum is about twice that of a 0.1-MeV proton.

4.6.8 The Bragg Curve


In reporting on his 1904 research on the ionization produced along the track of an alpha-particle, W.H.
Bragg plotted a graph of the ion pairs produced per unit distance as a function of the distance penetrated
by alpha particles in air. Known as the Bragg curve, this type of graph has been used countless times to
illustrate the concepts of range and stopping power. A Bragg ionization curve is the average distribution of
energy deposited, through ionization, per unit distance over the particle range and is described by
 ∞
i(r − s) −[(r−R)/α]2
I(s) = √ e dx, (4.153)
r α π

where α is the straggling parameter, i(r − s) is the specific ionization along the path of an individual particle
at a distance of (r − s), s is the penetration distance in the medium, r is the range of an individual particle,
and Rp is the average particle range.
144 Radiation Interactions in Matter Chap. 4

Figure 4.28. “Bragg curves” for alpha particles (helium nuclei) in silicon
showing the stopping power versus depth of penetration. Data obtained using
the SRIM program [Ziegler et al. 2013].

Closely related to the Bragg ionization curve is a graph of stopping power versus distance penetrated
along the track of an alpha particle or other charged particle. Examples are shown in Fig. 4.28, illustrating
energy loss along the tracks of alpha particles in silicon. In silicon, the stopping power is maximum for alpha
particles of energy about 460 keV. For alpha particles with initial energies above 460 keV, stopping power
increases along the particle path, reaches a maximum, and then decreases rapidly as the particle releases
most of its kinetic energy near the end of its path.

4.6.9 Approximate Range Formula for Charged Particles


An empirical mass range ρRCSDA for electrons, protons and alpha particles can be obtained by fitting the
equation
2
ρRCSDA (cm2 g−1 ) = 10a+bx+cx (4.154)
to calculated CSDA range data. Here x = log10 E with the initial energy E of the particle in units of MeV.
The empirical constants a, b, and c depend on the stopping material. This material dependence ameliorates
a deficiency of the empirical formula of Eq. (4.136) for the mean electron range. Values of a, b, and c for a
few materials are given in Table 4.3 for electrons and Table 4.4 for protons and alpha particles. Values of
these parameters for other materials can be obtained from the STAR computer code package [Berger 1992].
If computer codes, empirical data, and/or particles ranges, such as listed in Table 4.4, are not available,
then alternative relations do exist that can yield an acceptable result. For instance, from the analysis of
Bragg and Kleeman [1905], an expression is available for heavy ions as a ratio of ranges for monoenergetic
particles in different media 
R1 ρ2 A1
= , (4.155)
R2 ρ1 A2
where R1 and R2 are the ranges for alpha particles in two materials of density ρ1 and ρ2 , and atomic
masses A1 and A2 . Eq. (4.155) is commonly called the Bragg-Kleeman Rule, and is best used for materials
with similar atomic masses. The use of Eq. (4.155) is straightforward for elemental materials, but requires
Sec. 4.6. Charged-Particle Interactions 145

Table 4.3. Constants for the empirical formula of


Eq. (4.154). Valid for energies between 0.1 and 10
MeV.

Electrons

Material a b c

C -0.30434 1.2633 -0.21918


Al -0.25876 1.2380 -0.22597
Si -0.27136 1.2360 -0.22740
Ar -0.22887 1.2209 -0.23682
Ge -0.18537 1.2069 -0.23702
Ag -0.16377 1.1903 -0.24781
Xe -0.14796 1.1738 -0.25395
Pb -0.10787 1.1458 -0.25628
air -0.31149 1.2419 -0.23063
H2 O -0.36173 1.2587 -0.21600
LiF -0.26944 1.2572 -0.21674

Source: Fit to data from STAR codes [Berger 1992].

Table 4.4. Constants for the empirical formula y = a+bx+cx2 relating charged-particle
energy and its projected range, in which y is log10 of ρRCSDA (g/cm2 ) and x is log10 of
the initial particle energy Eo (MeV). Valid for energies between 0.1 and 10 MeV.

Protons Alpha Particles

Material a b c a b c

C -2.5542 1.4997 0.22046 -3.2132 1.0080 0.29815


Al -2.4108 1.4570 0.19861 -3.0581 .99132 0.27018
Si -2.4232 1.4802 0.17421 -3.0813 .98208 0.29625
Ar -2.3756 1.4944 0.16909 -3.0030 .93249 0.32566
Ge -2.2097 1.4045 0.17980 -2.7867 .96529 0.19442
Ag -2.1440 1.3815 0.18943 -2.7267 .95425 0.21643
Xe -2.1265 1.4375 0.13890 -2.7556 .97004 0.26094
Pb -1.9923 1.3663 0.17444 -2.5803 .98740 0.19178
air -2.5510 1.5066 0.21732 -3.1854 .94174 0.34192
H2 O -2.6144 1.4975 0.23219 -3.2357 .93102 0.33442
LiF -2.4883 1.4501 0.25453 -3.1240 .96343 0.30053

Source: Fit to data from STAR codes [Berger 1992].

a conversion to an effective atomic mass when used with mixtures and compounds [Henriksen and Baarli
1957]. There are various expressions for the effective atomic mass, some fairly complicated [see for example,
Birgani et al. 2012]. Offered here is a relatively simple variation [Birks 1964]
 &   2

Aeff = fi Ai fi Ai , (4.156)
i=1 i=1

where fi and Ai are the atomic fraction and atomic mass of element i. Knowledge of alpha particle range
data for one material will allow estimations of alpha particle ranges in another material.
146 Radiation Interactions in Matter Chap. 4

Example 4.1: Estimate the range in water of a 6-MeV triton (nucleus of 3 H). Data for the empirical
range formula of Eq. (4.154) are not provided for a triton. We must, therefore, estimate the triton’s range
from the observation that, for a given medium, the range R of heavy charged particles with the same speed
is proportional to m/z 2 , where m and z are the mass and charge of the particle.

Solution:
Step 1: First find the kinetic energy of a proton with the same speed as the 6-MeV triton. Classical
mechanics, appropriate for these energies, gives

Ep (1/2)mp vp2 mp 1
= = = .
ET (1/2)mT vT2 mT 3
The proton energy with the same speed as a 6-MeV triton is, thus, Ep = ET /3 = 2 MeV.
Step 2: Now we find the range in water of a 2-MeV proton using the empirical formula of Eq. (4.154) and
the data in Table 4.4. With x = log10 2 = 0.30103
2
ρRp (2 MeV) = 10−2.6144+1.4975x+0.23219x = 0.007202 g/cm2 .

Since ρ = 1 g/cm3 , Rp (2 MeV) = 0.007202 cm.


Step 3: From the range “rule” for the same medium (following Eq. (4.152)), we have

RT (6 MeV) mT zp2 31
= = = 3.
Rp (2 MeV) mp zT2 11
The range of the triton is then RT (6 MeV) = 3Rp (2 MeV) = 0.0216 cm.

Example 4.2: What is the range of 5.5 MeV alpha particles in silicon dioxide (SiO2 )?

Solution:
Step 1: Determine the effective atomic mass of SiO2 . From Eq. (4.156),
 2
 ' √
Aeff = fi Ai fi Ai
i=1 i=1
 ' √ √ 2
= fSi ASi + fO AO fSi ASi + fO AO
 ' √ √ 2
= 0.333(28) + .666(16) 0.333 28 + .666 16 = 20.38 g mol−1

Step 2: Determine the range of 5.5 MeV alpha particles in a material with similar atomic mass. Here, Si is
chosen for the material with a known range. From Eq. (4.154) and Table 4.4, with x = log10 5.5 = 0.7404,
2
ρRα (5.5 MeV) = 10−3.0813+0.98208(0.7404)+0.29625(0.7404) = 0.0064 g/cm2 .

The density of Si is 2.32 g cm−3 , yielding


0.0064
Rα (5.5 MeV) = = 0.00277 cm = 27.7 μm.
2.32
Sec. 4.6. Charged-Particle Interactions 147

Step 3: Use Eq. (4.155) to find the range in SiO2 (quartz). The density of quartz is 2.65 g cm−3 . Therefore,
 
2.32 g cm−3 20.38
RSiO2 = (0.00277 cm) = 0.0021 cm = 21 μm.
2.65 g cm−3 28
By comparison to the SRIM code [Ziegler et al. 2013], the answers are RSi = 28 microns and RSiO2 = 22
microns.

4.6.10 Range of Fission Fragments


The range of a fission fragment is difficult to calculate because the fission fragment’s charge changes as it
slows down. The lighter of the two fragments, having more initial kinetic energy, has a somewhat longer
range. An empirical formula with an accuracy of ±10% for the range (in units of mass thickness) of a fission
product, with initial kinetic energy E (in MeV), is [Alexander and Gazdik 1960]
EH,L
ρR (mg/cm2 )  C E 2/3 , ≤ E ≤ EH,L (4.157)
2
where EH,L refers to the initial energy of either the midpoint heavy or light fission fragment (nominally 67.9
MeV and 99.9 MeV, respectively), and


⎪ 0.14, air

0.19, aluminum
C= (4.158)

⎪ 0.27, nickel

0.50, gold
Measurements by Fulmer [1957] indicate slightly longer ranges than predicted by Eq. (4.157). Figures 4.29
and 4.30 demonstrate the residual energy after a fission fragment passes through a mass thickness ρR. The
x-axis intercept is the range of the fragment.
Heavy frag. energy (MeV)
Light frag. energy (MeV)

Figure 4.29. Energy of the median light fission Figure 4.30. Energy of the median heavy fis-
product (initial energy 99.9 MeV) after penetrat- sion product (initial energy 67.9 MeV) after
ing a distance R into various materials. After penetrating a distance R into various materi-
Fulmer [1957]. als. After Fulmer [1957].
148 Radiation Interactions in Matter Chap. 4

PROBLEMS
1. A broad beam of neutrons is normally incident on a homogeneous slab 6-cm thick. The intensity of
neutrons transmitted through the slab without interactions is found to be 30% of the incident intensity.
(a) What is the total interaction coefficient μt for the slab material? (b) What is the average distance
a neutron travels in this material before undergoing an interaction?
2. Based on the interaction coefficients tabulated in Appendix B, plot the tenth-thickness (in centimeters)
versus photon energy from 0.1 to 10 MeV for water, concrete, iron, and lead.

3. With the data of Table B.5, calculate the half-thickness for 1-MeV photons in (a) water, (b) iron, and
(c) lead.

4. A material is found to have a tenth-thickness of 2.3 cm for 1.25-MeV gamma rays. (a) What is the linear
attenuation coefficient for this material? (b) What is the half-thickness? (c) What is the mean-free-path
length for 1.25-MeV photons in this material?

5. Calculate the linear interaction coefficients in pure air at 20◦ C and 1 atm pressure for a 1-MeV photon
and a thermal neutron (2200 m s−1 ). Assume that air has the composition 75.3% nitrogen, 23.2%
oxygen, and 1.4% argon by mass. Use the following data:

Photon Neutron
2 −1
Element μ/ρ (cm g ) σtot (b)

Nitrogen 0.0636 11.9


Oxygen 0.0636 4.2
Argon 0.0574 2.2

6. In natural uranium, 0.720% of the atoms are the isotope 235 U, 0.0055% are 234 U, and the remainder
238
U. From the data in Table B.3, what is the total linear interaction coefficient (macroscopic cross
section) for a 2200 m s−1 neutron in natural uranium? What is the total macroscopic fission cross
section for 2200 m s−1 neutrons?

7. At a particular position, the flux density of particles is 2 × 1012 cm−2 s−1 . (a) If the particles are
photons, what is the density of photons at that position? (b) If the particles are thermal neutrons (2200
m/s), what is the density of neutrons?

8. A beam of 2-MeV photons with intensity 108 cm−2 s−1 irradiates a small sample of water. (a) How
many photon-water interactions occur in one second in one cm3 of the water? (b) How many positrons
are produced per second in one cm3 of the water?

9. A small homogeneous sample of mass m (g) with atomic mass A is irradiated uniformly by a constant
flux density φ (cm−2 s−1 ). If the total atomic cross section for the sample material with the irradiating
particles is denoted by σt (cm2 ), derive an expression for the fraction of the atoms in the sample that
interact during a 1-h irradiation. State any assumptions made.

10. A 1-mCi source of 60 Co is placed in the center of a cylindrical water-filled tank with an inside diameter
of 20 cm and depth of 100 cm. The tank is made of iron with a wall thickness of 1 cm. What is the
uncollided flux density at the outer surface of the tank nearest the source?
Problems 149

11. Derive the Compton formula, Eq. (4.32), given that the momentum of a photon
 of energy E is equal to
E/c and the momentum of an electron of kinetic energy T is equal to (1/c) T (T + 2me c2 ).
12. Verify Eqs. (4.34) to (4.39).
13. Verify Eq. (4.61); that is, given Eq. (4.63), carry out the integration

aσT (θs )
σT = dΩ .
4π dΩs

14. What is the maximum possible kinetic energy (keV) of a Compton electron and the corresponding
minimum energy of a scattered photon resulting from scattering of (a) a 100-keV photon, (b) a 1-MeV
photon, and (c) a 10-MeV photon? Estimate for each case the range the electron would have in air of
1.2 mg/cm3 density and in water of 1 g/cm3 density.
15. Compute and plot the energy spectrum F (T ) of Compton recoil electrons for incident photons of 0.5
and 2.0 MeV. Here F (T ) dT is the fraction of electrons with energies between T and T + dT .
16. Consider the classical mechanics of neutron inelastic scattering by a target atom initially at rest. Derive
Eq. (4.40), which relates the angle of scattering in the laboratory system and the neutron energies
before and after scattering. Suggestion: Apply the law of cosines to the triangle of Fig. 4.2(b). Note
that p2 = 2mE, (p )2 = 2mE  , p2r = 2M T , and T = E − E  + Q.
17. From Fig. 4.14, the total microscopic cross section in iron for neutrons with energy of 27 keV is about
0.4 b, and for a neutron with an energy of 28 keV about 90 b. (a) Estimate the fraction of 27-keV
neutrons that pass through a 10-cm thick slab without interaction. (b) What is this fraction for 28-keV
neutrons?
18. Consider the classical mechanics of neutron inelastic scattering by a target atom initially at rest. Derive
Eq. (4.47), which relates the angles of scattering in the laboratory and center-of-mass systems. Sugges-
tion: From Fig. 4.3(c) note that vc sin θc = v  sin θs , and vo + vc cos θc = v  cos θs . Apply trigonometric
identities and the definition γ ≡ vo /vc to reach the solution.
19. What is the maximum possible kinetic energy (keV) of a Compton electron and the corresponding
minimum energy of a scattered photon resulting from scattering of (a) a 100-keV photon, (b) a 1-MeV
photon, and (c) a 10-MeV photon? Estimate for each case the range the electron would have in air of
1.2 mg/cm3 density and in water of 1 g/cm3 density.
20. Consider the classical mechanics of neutron inelastic scattering by a target atom initially at rest. Derive
Eq. (4.49) for the ratio of the speed of the target atom before scatter to the speed of the neutron after
scatter. Show that for elastic scatter, γ = m/M = 1/A. Suggestion: Note that the total kinetic energy
relative to the center of mass is equal to the kinetic energy of the reduced mass μ ≡ mM/(M + m) =
mA/(1 + A) moving at the relative velocity between the neutron and atom. Note, too, that the kinetic
energy in the center-of-mass system after scatter differs from that before scatter by the Q value. That is,
  2  2
2 μ(vc + Vc ) = 2 μv + Q so that (vc ) = [2A/m(A + 1)][EA/(1 + A) + Q]. Similarly, (m + M )vo ≡ mv,
1 1 2
2 2
so that vo = 2E/m(A + 1) .
21. Consider the classical mechanics of neutron inelastic scattering by a target atom initially at rest. Derive
Eq. (4.50), which relates the angle of scattering in the center-of-mass system and the neutron energies
before and after scattering. Suggestion: Apply the law of cosines to Fig. 4.3c, with the result that
v 2 = (vc )2 + vo2 + 2vo vc ωc and apply the results of Problem 20 for vo and vc .
150 Radiation Interactions in Matter Chap. 4

22. Take as given that elastic scattering of neutrons by hydrogen atoms is isotropic in the center-of-mass
system. How would you determine the fraction of neutrons scattered at angles less than 45 degrees in
the laboratory system?

23. The differential scattering cross section (b/sr) for 1-MeV neutrons on Mg in the laboratory system is

dσs (E, ωs ) 2.7


= [1 + 1.2P1 (ωs ) + 0.75P2 (ωs ) + 0.08P3 (ωs )].
dΩs 4π
(a) Evaluate the total scattering cross section σs (E). (b) Evaluate the mean cosine of the laboratory
scattering angle ωs . (c) Evaluate the mean cosine of the center-of-mass scattering angle ωc . (d)
Evaluate the average energy lost by such neutrons in scattering. (e) Compute and plot versus ωc the
scattering cross section σs (E, ωc ) for such neutrons.

24. When an electron moving through air has 5 MeV of energy, what is the ratio of the rates of energy loss
by bremsstrahlung to that by collision? What is this ratio for lead?

25. About what thickness of aluminum is needed to stop a beam of (a) 2.5-MeV electrons, (b) 2.5-MeV
protons, and (c) 10-MeV alpha particles? Hint: For parts (a) and (b), use Tables 4.4 and 4.3 and
compare your values to ranges shown in Figs. 4.23 and (4.27). For part (c), use the range interpolation
rules on page 143.

26. Estimate the range of a 10-MeV tritium nucleus in air.

27. Verify that under the continuous slowing-down approximation for charged particles,

⊥ L(ro − r)
Fpl (r, E) = F (r, E) = ,
E/ro

in which L(ro − r) is the LET evaluated at the energy of the particle with residual CSDA range ro − r.

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Chapter 5

Sources of Radiation

I proposed the word radioactivity which has since become generally adopted;
the radioactive elements have been called radio elements.
Marie Curie

5.1 Introduction
In our world ionizing radiation is ever present, though rarely noticed by our human senses. It is with radiation
sensors that such radiation is detected and its characteristics measured. However, the type of sensor to use
depends on the type of radiation, its energy, and what information is sought about the radiation. In this book
many types of radiation detectors are discussed, each designed for specific types of radiation measurements.
Key to any radiation measurement is an understanding of the type and characteristics of the radiation being
measured. In this chapter, the most common sources of ionizing radiation are reviewed and many of their
properties examined. Much of the material presented here has been excerpted from expanded treatments
given in Shultis and Faw [2000] and Faw and Shultis [2012].

5.1.1 Origins of Ionizing Radiation


Ionizing radiation is invariably the consequence of physical reactions, involving subatomic particles, at the
atomic or nuclear level. The possible radiation-producing reactions are many and, usually, although not
always, involve altering the configuration of neutrons and protons in an atomic nucleus or the rearrangement
of atomic electrons about a nucleus. These radiation producing reactions can be divided into the following
two categories.
Radioactive Decay
In the first type of reaction, the nucleus of an atom spontaneously changes its internal arrangement of
neutrons and protons to achieve a more stable configuration. In such spontaneous radioactive transmutations,
ionizing radiation is almost always emitted. The number of known different atoms, each with a distinct
combination of Z and A, is about 3200. Of these, only 266 are stable and 65 are very long-lived radioisotopes
still found in nature. The remaining nuclides have been made by humans and are radioactive with lifetimes
much shorter than the age of the solar system. Both naturally occurring and manufactured radionuclides
are the most commonly encountered sources of ionizing radiation.
Binary Reactions
The second category of radiation-producing interactions involves two impinging atomic or subatomic particles
that react to form one or more reaction products. Examples include neutrons interacting with nuclei of
atoms, photons interacting with nuclei or atomic electrons, and cosmic rays interacting with nuclei in our
atmosphere. Such reactions invariably produce, as reaction products, ionizing radiation.

153
154 Sources of Radiation Chap. 5

5.1.2 Physical Characterization of Radiation Sources


The most fundamental type of source is a point source. Clearly no real source can have zero size, but a real
source can be approximated as a point source provided (1) that the volume is sufficiently small, that is, it
has dimensions much smaller than the dimensions of the attenuating medium between source and detector,
and (2) that there is negligible interaction of radiation with the matter in the source volume. The second
requirement may be relaxed if source characteristics are modified to account for source self-absorption and
other source-particle interactions.
In general, a point source may be characterized as depending on energy, direction, and time. In almost
all cases, time is not treated as an independent variable because the time delay between a change in the
emission rate of the source and the resulting change in the radiation field is usually negligible so that the
time dependence of the radiation field is that of the source.1 Therefore, the most general characterization
of a point source used here is in terms of energy and direction. Most radiation sources treated in radiation
measurements are isotropic, so that source characterization requires only knowledge of energy dependence.
Radioisotope sources are certainly isotropic, as are fission sources and capture gamma-ray sources.
Radiation sources may also be distributed along a line, over an area, or within a volume. Source charac-
terization requires, in general, spatial and energy dependence. Occasionally it is necessary to include angular
dependence. This is especially true for effective area sources associated with computed angular flows across
certain planes.
Energy dependence may be discrete, such as for radionuclide sources, or continuous, as for bremsstrahlung
or fission neutrons and photons. When discrete energies are numerous, an energy multigroup approach is
often used. The same multigroup approach may be used to approximately characterize a source whose
emissions are continuous in energy.

5.2 Sources of Gamma Rays


Radioactive sources abound in our technological age and are used for a wide variety of purposes in many
educational, medical, research, industrial, governmental, and commercial facilities. The radionuclides in these
sources almost always leave their progeny in excited nuclear states whose subsequent transitions to lower-
energy states usually result in the emission of one or more gamma photons. Consequently, these radioactive
sources are frequently encountered in radiation measurements and in verifying the proper operation of a
radiation detector.
In characterizing the gamma radiation emitted by a radioactive source, a careful distinction must be
made between the activity of a radioisotope and its source strength. Activity is precisely defined as the
expected number of atoms undergoing radioactive transformation per unit time. The SI unit of activity
is the becquerel (Bq), equivalent to 1 transformation per second, while the older unit for activity is the
curie (Ci) equal to 3.7 × 1010 transformations per second. Activity is not defined as the number of particles
emitted per unit time, and the decay of two common laboratory radioisotopes, 60 Co and 137 Cs, can be used
to illustrate this point. Each transformation of 60 Co results in the emission of two gamma rays, one at 1.173
MeV and the other at 1.333 MeV. However, each transformation of 137 Cs, accompanied by a transformation
of its decay product 137m Ba, results in emission of a 0.662-MeV gamma ray with an 85% probability.
Extensive compilations of the energies and intensities of the gamma and x rays emitted by radionuclides
are available, for example [Kocher 1981; ICRP 1983; Weber et al. 1989; Eckerman et al. 1994], or computer
programs that can be used to prepare specialized compilations [Dillman 1980]. Especially useful is the on-line
decay data base for radionuclides that is found at https://www.nndc.bnl.gov/nudat2.

1 Exceptions include nuclear explosions or supernovae where the radiation field is very far from the source.
Sec. 5.2. Sources of Gamma Rays 155

5.2.1 Naturally Occurring Radionuclides


Radionuclides existing on earth arise from two sources. First, earth has always been bombarded by cosmic
rays coming from the sun and from intergalactic space. For the most part, cosmic rays consist of protons
and alpha particles, with heavier nuclei contributing less than 1% of the incident nucleons.2 These cosmic
rays interact with atoms in the atmosphere and produce a variety of light radionuclides.
The second source of naturally occurring radionuclides is the residual radioactivity in the matter from
which the earth was formed. These heritage or primordial radionuclides were formed in the stars from whose
matter the solar system was formed. Most of these radionuclides have long since decayed away during the 4
billion years since the earth was formed.
When making measurements of a gamma-ray source, there is always a background source of radiation
as a consequence of the ubiquitous presence of naturally occurring radionuclides. Here the major sources of
such radionuclides are discussed.
Cosmogenic Radionuclides
Cosmic rays interact with constituents of the atmosphere, sea, or earth, but mostly with the atmosphere,
leading directly to radioactive products. Capture of secondary neutrons produced in primary interactions of
cosmic rays leads to many more. Only those produced from interactions in the atmosphere lead to significant
radiation exposure to humans.
The most prominent of the cosmogenic radionuclides are tritium 3 H and 14 C. The 3 H (symbol T or t)
is produced mainly from the 14 N(n,T)12 C and 16 O(n,T)14 N reactions. Tritium has a half-life of 12.3 years
and, upon decay, emits one β − particle with a maximum energy of 18.6 (average energy 5.7) keV. Tritium
exists in nature almost exclusively as HTO.3
The nuclide 14 C is produced mainly from the 14 N(n, p)14 C reaction. It exists in the atmosphere as CO2 ,
but the main reservoirs are the oceans. 14 C has a half-life of 5730 years and decays by β − emission with a
maximum energy of 157 keV and average energy of 49.5 keV.
Over the past century, combustion of fossil fuels with the emission of CO2 without any 14 C has diluted
the cosmogenic content of 14 C in the environment. Moreover, since the use of nuclear weapons in World War
II, artificial introduction of 3 H and 14 C (and other radionuclides) by human activity has been significant,
especially from atmospheric nuclear-weapons tests. Consequently, these isotopes no longer exist in natural
equilibria in the environment.
Singly Occurring Primordial Radionuclides
Of the many radionuclide species present when the solar system was formed 4.57 billion years ago, some 17
very long-lived radionuclides still exist as singly occurring or isolated radionuclides, that is, as radionuclides
not belonging to a radioactive decay chain. These radionuclides are listed in Table 5.1, and all but one are
seen to have half-lives greater than the age of the solar system. Of these radionuclides, the most significant
(from a human exposure perspective) are 40 K and 87 Rb because they are inherently part of our body tissue.
Decay Series of Primordial Origin
Each naturally occurring radioactive nuclide with Z > 83 is a member of one of three long decay chains,
or radioactive series, stretching through the upper part of the Chart of the Nuclides. These radionuclides
decay by α or β − emission and they have the property that the number of nucleons (mass number) A for
each member of a given decay series can be expressed as 4n + i, where n is an integer and i is a constant (0,
2, or 3) for each series. The three naturally occurring series are named the thorium (4n), uranium (4n + 2),

2 Electrons,
primarily from the sun, also are part of the cosmic rays incident on the earth. But they are deflected by earth’s
magnetosphere and do not produce cosmogenic radionuclides.
3 H O with one hydrogen replaced by tritium.
2
156 Sources of Radiation Chap. 5

Table 5.1. The 17 isolated primordial radionuclides. Data taken from GE-NE [1996].

Radionuclide Half-life % El. Radionuclide Half-life % El.


& the Decay Modes (years) Abund. & the Decay Modes (years) Abund.
40 K β − EC β + 1.27 × 109 0.0117 50 V β − EC 1.4 × 1017 0.250
19 23
87 Rb β− 4.88 × 1010 27.84 113 Cd β− 9× 1015 12.22
37 48
115 In β− 4.4 × 1014 95.71 123 Te EC > 1.3 × 1013 0.908
49 52
138 La EC β − 1.05 × 1011 0.090 144 Nd α 2.38 × 1015 23.80
57 60
147 Sm α 1.06 × 1011 15.0 148 Sm α 7× 1015 11.3
62 62
152 Gd α 1.1 × 1014 0.20 176 Lu β− 3.78 × 1010 2.59
64 71
174 Hf α 2.0 × 1015 0.162 180 Ta EC β+ > 1.2 × 1015 0.012
72 73
187 Re β− 4.3 × 1010 62.60 186 Os α 2 × 1015 1.58
75 76
190 Pt α 6.5 × 1011 0.01
78

Table 5.2. Principal radioisotopes in two naturally occurring pri-


mordial decay series. Source: NUDAT 2.5, National Nuclear Data
Center, Brookhaven National Laboratory.

Thorium Series Uranium Series

Nuclide & Half-lifea Nuclide & Half-lifea


decay mode T1/2 decay mode T1/2
232 Th α 14.05 Gy 238 U α 4.468 Gy
90 92
228 Ra β 5.75 y 234 Th β 24.10 d
88 90
228 Ac β 6.15 h 234m Pa β 1.159 m
89 91
228 Th α 1.912 y 234 U α 244.5 ky
90 92
224 Ra α 3.66 d 230 Th α 75.4 ky
88 90
220 Rn α 55.6 s 226 Ra α 1600 y
86 88
216 Po α 0.145 s 222 Rn α 3.8235 d
84 86
212 Pb β 10.64 h 218 Po α, β 3.098 m
82 84
212 Bi α, β 60.55 m 218 At α 1.5 s
83 85
212 Po α 0.299 μs 214 Pb β 26.8 m
84 82
208 Tl β 3.053 m 214 Bi α, β 19.9 m
81 83
208 Pb ∞ 214 Po α 164 μs
82 84
210 Tl β 1.3 m
81
210 Bi α, β 5.012 d
83
210 Pb α, β 22.2 y
82
210 Po α 138.4 d
84
206 Hg β 8.2 m
80
206 Tl β 4.2 m
81
206 Pb ∞
82
a Gy = 109 y, ky = 103 y, μs = 10−6 s.
Sec. 5.2. Sources of Gamma Rays 157

and actinium (4n + 3) series, named after the radionuclide at, or near, the head of the series. The head of
each series has a half-life much greater than any of its daughters.
There is no naturally occurring series represented by 4n + 1. This series was recreated after 241 94 Pu was
made in nuclear reactors. This series does not occur naturally since the half-life of the longest lived member
93 Np, is only 2.14 × 10 y, much shorter than the age of the earth (4.54 × 10 y). Hence, any
of the series, 237 6 9

members of this series that were in the original material of the solar system have long since decayed away.
The principal radioisotopes produced by the two most important naturally occurring series (the uranium
and thorium series) are given in Table 5.2. In both of these decay chains, a few members decay by both
α and β − decay causing the decay chain to branch (see Shultis and Faw [2000]). Nevertheless, each decay
chain ends in the same stable isotope.

5.2.2 Prompt Fission Gamma Photons


Whenever a heavy nucleus fissions, copious gamma photons are produced either within the first 6 × 10−8 s
after the fission event (the prompt fission gamma photons) or from the subsequent decay of the fission
products. If radiation measurements are being made in the presence of fission sources, for example, these
prompt and delayed gamma rays are of great importance.
Most investigations of prompt fission gamma photons have centered on the thermal-neutron-induced
fission of 235 U. For this nuclide it has been found that the number of prompt fission photons is 8.13 ± 0.35
photons per fission over the energy range 0.1 to 10.5 MeV, and the energy carried by this number of photons
is 7.25 ± 0.26 MeV per fission [Keepin 1965]. The energy spectrum of prompt gamma photons from the
thermal fission of 235 U between 0.1 and 0.6 MeV is approximately constant at 6.6 photons MeV−1 fission−1 .
At higher energies the spectrum falls off sharply with increasing energy. The measured energy distribution
of the prompt fission photons can be represented by the following empirical fit over the range 0.1 to 10.5
MeV [Keepin 1965]: ⎧

⎪ 6.6 0.1 < E < 0.6 MeV

N (E) = 20.2e−1.78E 0.6 < E < 1.5 MeV



7.2e−1.09E 1.5 < E < 10.5 MeV,
where E is in MeV and N (E) is in units of photons MeV−1 fission−1 .
Investigation of 233 U, 239 Pu, and 252 Cf indicates that the prompt fission photon energy spectra for these
isotopes resembles very closely that for 235 U, and hence for most purposes it is reasonable to use the 235 U
spectrum for other fissioning isotopes.

5.2.3 Fission-Product Gamma Photons


With the widespread application of nuclear fission, an important concern is the consideration of the very long
lasting gamma-ray activity produced by the decay of fission products. In the fission process, most often two
fragments are produced (binary fission). About 0.3% of the time a third light fragment is produced (ternary
fission), most often 3 H. The mass distribution or fission-product chain yield is bi-modal, with many products
having atomic mass number around 95 and around 140. Among the former are the important long-lived
radionuclide 90 Sr, several isotopes of the halogen bromine, and various isotopes of the noble gas krypton.
Among the heavy fragments are the important long-lived radionuclide 137 Cs, radioisotopes of halogen iodine,
notably 131 I, and isotopes of the noble gas xenon. The fission-products are neutron-rich and decay almost
exclusively by β − emission, often forming long decay chains. From the range of mass numbers produced,
about 100 different decay chains are formed. An example of a short chain is
β− β− β− β−
140
54 Xe −→ 140
55 Cs −→ 140
56 Ba −→ 140
57 La −→ 140
58 Ce (stable).
16 s 66 s 12.8 d 40 h
158 Sources of Radiation Chap. 5

The total gamma-ray energy released by the fission product chains is comparable to that released as
prompt fission gamma photons. The gamma-ray energy release rate declines rapidly with time after fission.
About three-fourths of the delayed gamma-ray energy is released in the first thousand seconds after fission.
In most calculations involving spent nuclear fuel, the gamma activity at several months or even years after
removal of fuel from the nuclear reactor is of interest and so only the long-lived fission products need be
considered.
It has been found that the gamma energy released from fission products is relatively independent of the
energy of the neutrons causing the fissions. However, the gamma-ray energy released and the photon energy
spectrum depend significantly on the fissioning isotope, particularly in the first 10 s after fission. Generally,
fissioning isotopes, having a greater proportion of neutrons to protons, produce fission-product chains of
longer average length, with isotopes richer in neutrons and hence with greater available decay energy. Also,
the photon energy spectrum generally becomes less energetic as the time after fission increases.
The delayed gamma photon energy spectrum from the fission of 235 U, at times up to about 5 s, may be
approximated by the proportionality
N (E) ∼ e−1.1E , (5.1)

where N (E) is the delayed gamma-ray yield (photons MeV−1 fission−1 ) and E is the photon energy in MeV.
The time dependence for the total gamma photon energy emission rate F (t) (MeV s−1 fission−1 ) is often
described by the simple decay formula

F (t) = 1.4t−1.2 , 10 s < t < 107 s, (5.2)

where t is in seconds. More complicated (and accurate) expressions for F (t) have been obtained from fits to
experimental data (see, for example, Shultis and Faw [2000]); but for preliminary calculations the simpler
result is usually adequate. It is observed that both 235 U and 239 Pu have roughly the same total gamma-
ray-energy decay characteristics for up to 200 days after fission, at which time 235 U products begin to decay
more rapidly. At 1 year after fission, the 239 Pu gamma-ray emission rate is about 60% greater than that of
235
U.
For accurate calculations involving fission products, the variation with time after fission of the energy
spectra of the photons must be taken into account. Often the energy spectra are averaged over discrete
energy intervals and the energy emission rate in each energy group is considered as a function of time after
fission. Computer codes, based on extensive libraries of radionuclide data, have been developed to compute
the abundances and decay rates of the hundreds of fission-product radionuclides. One such code is ORIGEN
[Hermann and Westfall 1981; RSIC 1991].

5.2.4 Capture Gamma Photons


The compound nucleus formed by neutron absorption is initially created in a highly excited state with
excitation energy equal to the kinetic energy of the incident neutron plus the neutron binding energy, which
averages about 7 MeV. The decay of this nucleus, usually within 10−12 s, and usually by way of intermediate
states, typically produces several energetic photons. Generally, the probability a neutron causes an (n, γ)
reaction is greatest for slow moving thermal neutrons, i.e., neutrons whose speed is in equilibrium with the
thermal motion of the atoms in a medium. At high energies, it is more likely that a neutron scatters, thereby
losing some of its kinetic energy and, thus, slows towards thermal energies. Table B.4 in Appendix B lists
the number of capture gamma photons by 1-MeV energy bin when a thermal neutron is absorbed in various
elements
Capture photons may be created intentionally by placing a material with a high thermal-neutron (n, γ)
cross section in a thermal neutron beam. The energy spectrum of the resulting capture gamma photons can
Sec. 5.3. Sources of X Rays 159

then be used to identify trace elements in the sample. More often, however, capture gamma photons are an
undesired secondary source of radiation.
The absorption of a thermal neutron by an isotope or element typically produces dozens of capture
photons, each with a unique energy and probability of emission. Detailed compilations of the energies and
frequencies are provided by Révay et al. [2004]. Analysis of the capture gamma photon spectrum emitted
by an unknown sample can be used to infer the elemental composition of the sample. Generally, only a few
of the most intense capture photons for a particular element are needed. In Table B.5 (Appendix B), the
energies of the three capture photons recommended for each element for elemental identification are given.

5.2.5 Inelastic Scattering Gamma Photons


The excited nucleus formed when a neutron is inelastically scattered decays to the ground state usually
within about 10−14 s, with the excitation energy being released by one or more photons. Because of the
constraints imposed by the conservation of energy and momentum in all scattering interactions, inelastic
neutron scattering cannot occur unless the incident neutron energy is greater than (A + 1)/A times the
energy required to excite the scattering nucleus to its first excited state (see Section 4.3.5). Except for the
heavy nuclides, neutron energies above about 0.5 MeV are typically required for inelastic scattering.
The detailed calculation of secondary photon source strengths from inelastic neutron scattering requires
knowledge of the fast-neutron flux, the inelastic scattering cross sections, and spectra of resultant photons, all
as functions of the incident neutron energy. The cross sections and energy spectra of the secondary photons
depend strongly on the incident neutron energy and the particular nuclide. Such inelastic scattering data
are known only for the more important structural and shielding materials, and even the known data require
extensive data libraries. Often inelastic scattered gamma rays are ignored in routine radiation measurements.
But in some cases their identification is vital because, from their energies and intensities, isotopic abundances
of a sample can be inferred.

5.2.6 Activation Gamma Photons


For many materials, absorption of a neutron or a proton produces a radionuclide with a half-life ranging
from a fraction of a second to many years. Many radionuclides encountered in research laboratories, medical
facilities, and industry are produced as activation nuclides from neutron or proton absorption in some
parent material (see Table 5.3). Such nuclides decay, usually by beta emission, leaving the daughter nucleus
in an excited state which usually decays quickly to its ground state with the emission of one or more gamma
photons. Thus, the apparent half-life of the photon emitter is that of the parent (or activation nuclide), while
the number and energy of the photons are characteristic of the nuclear structure of the decay daughter.

5.2.7 Positron Annihilation Photons


Positrons, generated either from the positron decay of radionuclides or from pair production interactions
induced by high energy photons, slow down in matter within about 10−10 s and are subsequently annihilated
with ambient electrons. With rare exception, the rest-mass energy of the electron and positron is emitted in
the form of two annihilation photons, each of energy me c2 (= 0.511 MeV).

5.3 Sources of X Rays


The interaction of photons or charged particles with matter leads inevitably to the production of secondary
x-ray photons which have energies < ∼ 100 keV. Because the energies of the x rays are unique to the element
that emits them, their energies and intensities can be used to determine the elemental composition of an
irradiated sample. For measurements of these x rays it is necessary to understand how the x rays are produced
and some characteristics of the production mechanisms. There are two principal methods whereby secondary
160 Sources of Radiation Chap. 5

Table 5.3. Important radioisotopes produced by reactors and accelerators


for use in medical, research, and industrial applications. Those isotopes
commercially available for medical use are shown in bold. Sources: Ref-
erences [4] and [5]. Decay data from NUDAT 2.5, National Nuclear Data
Center, Brookhaven National Laboratory.

Half- Decay Half- Decay


Nuclide Nuclide
life modesa life modesa
3H 12.33y β− * 81m Kr 13.1s EC IT
11 C 20.39m β + EC 85 Kr 10.76y β−
13 N 9.965m β + EC 82 Srb 25.6d EC *
14 C 5730y β− * 89 Sr 50.6d β−
15 O 122.2s β + EC 90 Src 28.90y β− *
18 F 109.8m β + EC 99 Mod 65.94h β−
22 Na 2.603y β + EC 103 Pd 16.99d EC
26 Al 7.17E5y β + EC 110m Ag 249.8d β − IT
28 Mg 20.91h β− 111 In 2.80d EC
32 Si 153y β− * 113m In 99.48m IT
32 P 14.26d β− * 123 I 13.2h EC
33 P 25.3d β− * 125 I 59.40d EC
35 S 87.51d β− * 131 I 8.052d β−
36 Cl 3.01E5y β ± EC 133 Xe 5.243d β−
46 Sc 83.79d β− 137 Cse 30.0y β− *
51 Cr 27.70d EC 140 La 1.679d β−
54 Mn 312.1d β− EC 148 Gd 74.6y α*
57 Co 271.7d EC 153 Sm 46.3h β−
57 Cu 196ms β + EC 159 Gd 18.48h β−
57 Cr 21.1s β− 169 Yb 32.02d EC
59 Fe 44.50d β− 170 Tm 128.6d β − EC
60 Co 5.271y β− 186 Re 89.25h β − EC
64 Cu 12.70h β ± EC 191 Os 15.4d β−
65 Zn 244.1d β + EC 192 Ir 73.83d β − EC
67 Ga 3.261d EC 198 Au 2.696d β−
68 Ga 67.71m β + EC 201 Tl 73.0h EC
75 Se 119.8d EC 204 Tl 3.78y β − EC *
81 Rb 4.572h β+ EC 210 Pb 22.2y β−
82 Rb 1.273m β+ EC 241 Am 432.6 y α
a Decays without any gamma photon emission are denoted by *.
b In equilibrium with decay product 82 Rb (1.273 m, β + EC).
c In equilibrium with decay product 90 Y (64.00 h, β − ).
d In equilibrium with decay product 99m Tc (6.01 h, IT).
e In equilibrium with decay product 137m Ba (2.552 m, IT).
Sec. 5.3. Sources of X Rays 161

x-ray photons are generated: the rearrangement of atomic electron configurations leads to characteristic x
rays, and the deflection of charged particles in the nuclear electric field results in bremsstrahlung. Both
mechanisms are discussed below.

5.3.1 Characteristic X Rays


The electrons around a nucleus are arranged in shells or layers, each of which can hold a maximum number
of electrons (see Section 3.4.6). The two electrons in the innermost shell (K shell) are the most tightly
bound, the six electrons in the next shell (L shell) are the next most tightly bound, and so on outward for
the M , N ,... shells. If the normal electron arrangement around a nucleus is altered through ionization of an
inner electron or through excitation of electrons to higher energy levels, the electrons begin a complex series
of transitions to vacancies in the lower shells (thereby acquiring higher binding energies) until the unexcited
state of the atom is achieved. In each electronic transition, the difference in binding energy between the final
and initial states is either emitted as a photon, called a characteristic x ray, or given up to an outer-shell
electron which is ejected from the atom, called an Auger electron. The discrete electron energy levels and
the transition probabilities between levels vary with the Z number of the atom and, thus, the characteristic
x rays provide a unique signature for each element.
The number of x rays with different energies is greatly increased by the multiplicity of electron energy
levels available in each shell (1, 3, 5, 7,... distinct energy levels for the K, L, M , N ,... shells, respectively).
To identify the various characteristic x rays for an element, many different schemes have been proposed.
One of the more popular uses the letter of the shell whose vacancy is filled together with a numbered Greek
subscript to identify a particular electron transition (e.g., Kα1 and Lγ5 ). In Fig. 5.1 the electron-energy-level
diagram is shown for lead, and the more probable and energetic transitions are indicated together with the
nomenclature for the associated characteristic x rays. The notation shown in this example is valid for any
element; that is, Kβ1 refers to the characteristic x ray produced when an electron from the third energy
level of the M shell fills a vacancy in the K shell. Fortunately, in many radiation measurements such detail
is seldom needed, and often only the dominant K series of x rays is considered, with a single representative
energy being used for all x rays.

Production of Characteristic X Rays


There are several methods commonly encountered in radiation measurement applications whereby atoms
may be excited and characteristic x rays produced. A photoelectric absorption leaves the absorbing atom in
an ionized state. If the incident photon energy is sufficiently greater than the binding energy of the K-shell
electron, which ranges from 14 eV for hydrogen to 115 keV for uranium, it is most likely (80 to 100%) that
a vacancy is created in the K shell and thus that the K series of x rays dominates the subsequent secondary
radiation. These x-ray photons produced from photoelectric absorption are often called fluorescent radiation
and are widely used to identify trace elements in a sample by bombarding the sample with low-energy
photons from a radioactive source or with x rays from an x-ray machine and then observing the induced
fluorescent radiation.
Characteristic x rays can also arise following the decay of a radionuclide. In the decay process known
as electron capture, an orbital electron, most likely from the K shell, is absorbed into the nucleus, thereby
decreasing the nuclear charge by one unit. The resulting K-shell vacancy then gives rise to the K series
of characteristic x rays. A second source of characteristic x rays, which occurs in many radionuclides, is a
result of internal conversion. Most daughter nuclei formed as a result of any type of nuclear decay are left in
excited states. This excitation energy may be either emitted as a gamma photon or transferred to an orbital
electron which is ejected from the atom. Again it is most likely that a K-shell electron is involved in this
internal conversion process.
162 Sources of Radiation Chap. 5

Figure 5.1. X-ray energy-level diagram for lead (Z = 82) showing the principal characteristic
x-ray transitions and their standard nomenclature. After Flügge [1957].

Energies of Characteristic X Rays


To generate a particular series of characteristic x rays, an electron vacancy must be created in an appropriate
electron shell. Such vacancies are created only when sufficient energy is transferred to an electron in that
shell so as to allow it to break free of the atom or at least be transferred to an energy level above all the other
electrons. In Chapter 4 it was seen that the photoelectric cross section changed abruptly at well-defined
energies, called edge energies, corresponding to the ionization or binding energy for electrons in the various
shells. Below the edge energy for a shell, vacancies can no longer be created in the shell and the photoelectric
cross section, therefore, is smaller because fewer electrons are now available to interact with the incident
photon. These shell edge energies increase with the atomic number Z of the atom as a result of the electrons
becoming more tightly bound in the atom. The edge energies or ionization energies for different shells and
even for the different electron states within the same shell can be found in many books on x-ray analysis [e.g.,
Flügge 1957], and in photon data libraries [e.g., Trubey et al. 1989]. A reasonably accurate approximation
Sec. 5.3. Sources of X Rays 163

Table 5.4. Values of the constants a b and c used to express principal


characteristic x-ray energies and the K-edge energy as E = aZ c exp(−bZ 3 ).
Maximum error is less than 100 eV, and mostly less than 30 eV.

X Ray or Edge a (eV) b c Fit Range

K-edge 6.85198 1.168 × 10−7 2.13240 7 < Z < 95


Kα1 7.51002 1.489 × 10−7 2.07109 7 < Z < 95
Kα2 7.63540 1.079 × 10−7 2.06582 7 < Z < 95
Kβ1 7.37998 1.208 × 10−7 2.10694 7 < Z < 95
Kβ2 6.95769 1.138 × 10−7 2.12778 7 < Z < 95
Kβ3 7.39760 1.116 × 10−7 2.10624 7 < Z < 95
Lα1 0.34810 −8.338 × 10−8 2.35265 30 < Z < 95
Lα2 0.35173 −9.667 × 10−8 2.34975 30 < Z < 95
Lβ1 0.31810 1.514 × 10−7 2.38418 30 < Z < 95
Lβ2 0.21302 −1.346 × 10−7 2.51145 30 < Z < 95

for the K-edge energy is


EK (eV) = a Z c exp[−bZ 3 ], (5.3)
where the parameters for a, b, and c are listed in Table 5.4.
The characteristic x rays emitted when electrons fill a vacancy in a shell always have less energy than that
required to create the vacancy. Extensive tabulations of characteristic x-ray energies are available [ICRP
1983; Weber et al. 1989; Eckerman et al. 1994]. From these results it is seen that the Kα x-ray energy varies
from only 0.52 keV for oxygen (Z = 8) to 6.4 keV for iron (Z = 26) to 98 keV for uranium (Z = 92). By
comparison, the L series of x rays for uranium occurs at energies around 15 keV.
Intensity of Characteristic X Rays
The fluorescent yield of a material is the fraction of the atoms with a vacancy in an inner electron shell
that emit an x ray upon the filling of the vacancy. Values for the fluorescent yield are found in Browne and
Firestone [1986] or in nuclear data libraries such as Eckerman et al. [1994]. For vacancies in the K shell, the
fluorescent yield can be approximated for 1 < Z < 100 by [Hubbell 1989]

B4
ωK = , (5.4)
1 + B4
where the parameter B is given by

B = 0.0370 + 0.03112Z + 5.44 × 10−5 Z 2 − 1.250 × 10−6 Z 3 . (5.5)

From the results of Eqs. (5.4) and (5.5) it is seen that the fluorescent yield increases dramatically with the
Z number, varying from 0.0069 for oxygen (Z = 8) to 0.97 for uranium (Z = 92). Thus, the secondary
fluorescent radiation is of more concern for heavy materials.

5.3.2 Bremsstrahlung
A charged particle gives up its kinetic energy either by collisions with electrons along its path or by photon
emission as it is deflected, and hence accelerated, by the electric fields of nuclei. The photons produced by
the deflection of the charged particle are called bremsstrahlung (literally, “braking radiation”). For a given
type of charged particle, the radiative stopping power, Lrad , increases with the particle energy and with the
square of the atomic number (Z) of the absorber [see Eq. (4.134)], while the collisional (ionization) stopping
power, Lcoll , decreases with particle energy and increases only with the first power of Z [see Eq. (4.131)].
164 Sources of Radiation Chap. 5

For a relativistic particle of rest mass M (i.e., E M c2 ) it can be shown that the ratio of radiative to
ionization losses is approximately [Evans 1955]
Lrad EZ me 2
 , (5.6)
Lcoll 700 M
where E is in MeV. From this result it is seen that bremsstrahlung is more important for high energy
particles of small mass incident on high-Z material. In most radiation measurement situations, only electrons
(me /M = 1) are ever of importance for their associated bremsstrahlung. All other charged particles are far
too massive to produce significant amounts of bremsstrahlung. Bremsstrahlung from electrons, however, is
of particular radiological interest for devices that accelerate electrons, such as betatrons and x-ray tubes, or
for situations involving radionuclides that emit only beta particles.
Thick-Target Bremsstrahlung for Monoenergetic Electrons
The energy distribution of the photons produced by the bremsstrahlung mechanism is continuous up to a
maximum energy corresponding to the maximum kinetic energy of the incident charged particles. The exact
shape of the continuous bremsstrahlung spectrum depends on many factors, including the energy distribution
of the incident charged particles, the thickness of the target, and the amount of bremsstrahlung absorbed in
the target and other masking material.
For monoenergetic electrons of energy Eo incident on a target thicker than the electron range, the number
of bremsstrahlung photons of energy E, per unit energy and per incident electron, emitted as the electron is
completely slowed down can be approximated by the distribution [Wyard 1952]
   
Eo 3 Eo
Nbr (Eo , E) = 2kZ − 1 − ln , E ≤ Eo , (5.7)
E 4 E
where k is a normalization constant independent of E. The fraction of the incident electron’s kinetic energy
that is subsequently emitted as bremsstrahlung can then be calculated from this approximation as
 Eo
1 5
Y (Eo ) = dE ENbr (Eo , E) = kZEo , (5.8)
Eo 0 8
which is always a small fraction in most situations. For example, only 4% of the energy of a 0.5-MeV
electron, when stopped in lead, is converted into bremsstrahlung. Equation (5.8) can be used to express
the normalization constant k in terms of Y (Eo ), namely kZ = 8Y (Eo )/(5Eo ). With this choice for k, the
approximation of Eq. (5.7) agrees quite well with the thick-target bremsstrahlung spectrum calculated by
much more elaborate methods, such as the continuous slowing-down model (see Fig. 5.2).
The angular distribution of bremsstrahlung is generally quite anisotropic and varies with the incident
electron energy. Bremsstrahlung induced by low-energy electrons (< ∼ 100 keV) is emitted predominantly
at 90◦ to the direction of the incident electron. As the electron energy increases, the direction of the
peak intensity shifts increasingly toward the forward direction, until for electrons above a few MeV, the
bremsstrahlung is confined to a very narrow forward beam [NCRP 1977]. The angular distribution of
radiation leaving a target is very difficult to compute since it depends on the target size and orientation. For
thin targets the anisotropy of the bremsstrahlung resembles that for a single electron-nucleus interaction,
while for thick targets multiple electron interactions and photon absorption in the target must be considered.
Bremsstrahlung from Beta Particles
The electrons and positrons emitted by radionuclides undergoing beta decay produce bremsstrahlung as they
slow down in the source material. In beta decay, the electrons or positrons are emitted with a continuous
distribution of energies from zero to a maximum energy Emax . The shape of the spectrum is a complicated
Sec. 5.3. Sources of X Rays 165

Figure 5.2. Distribution of bremsstrahlung photons, Nbr (Eo , E), produced by mo-
noenergetic electron beams (energy Eo ) incident on a thick lead target. The solid
lines are calculations based on the continuous slowing-down approximation (CSDA)
and the dashed lines are based on the Wyard approximation of Eq. (5.7).

function of the quantum mechanical properties of the parent nucleus (see Section 5.5.1), although computer
codes are available to calculate the beta spectrum for most radionuclides [Dillman 1980]. If the number of
beta particles emitted in unit energy about E (normalized to one electron) is denoted by Nβ (E), the energy
distribution Nbr (E  ) of the resulting bremsstrahlung intensity produced in a target thicker than the range
of the most energetic beta particles can be computed from Eq. (5.7) as
 Emax
Nbr (E  ) = dE Nβ (E)Nbr (E, E  ). (5.9)
E

This energy distribution of bremsstrahlung from beta decay is quite different from that from monoenergetic
electrons, the former being much softer and comparatively less intense at higher energies for Emax = Eo .
The average fraction of the beta-particle energy that is emitted as bremsstrahlung is
 Emax & Emax
fβ = dE E Y (E)Nβ (E) dE E Nβ (E). (5.10)
0 0
166 Sources of Radiation Chap. 5

Table 5.5. Characteristic X-ray properties of target materials used in


X-ray tubes.
X-ray Wavelength Energy Excitation
Element
line (10−10 m) (keV) voltage (kV)
Tungsten Kα1 0.2090 59.3182 69.525
Kβ1 0.1844 67.2443 69.525
Lα1 1.4764 8.3976 10.207
Lβ1 1.2818 9.6724 11.514
Silver Kα1 0.5594 22.1629 25.514
Lα1 4.1544 2.9843 3.351
Molybdenum Kα1 0.7093 17.4793 20.000
Kβ1 0.6323 19.6083 20.000
Lα1 5.4066 2.2932 2.520
Copper Kα1 1.5406 8.0478 8.979
Kβ1 1.3922 8.9053 8.979
Nickel Kα1 1.6579 7.4782 8.333
Cobalt Kα1 1.7890 6.9303 7.709
Iron Kα1 1.9360 6.4038 7.112
Chromium Kα1 2.2897 5.4147 5.989
Aluminum Kα1 8.3393 1.4867 1.560

Inner Bremsstrahlung
During the beta-decay process, the beta particle is accelerated by the positive charge of the nucleus, and
consequently, a small amount of bremsstrahlung is emitted. These x rays, called “inner” bremsstrahlung,
can usually be ignored because only a small fraction of the beta-decay energy, on the average, is emitted as
this type of radiation.

5.3.3 X-Ray Machines


The production of x-ray photons as bremsstrahlung and fluorescence occurs in any device that produces high
energy electrons. Devices that can produce significant amount of x rays are those in which a high voltage is
used to accelerate electrons, which then strike an appropriate target material. Such is the basic principle of
all x-ray tubes used in medical diagnosis and therapy, industrial applications, and research laboratories.
Although there are many different designs of x-ray sources for different applications, most designs for low
to medium voltage sources (< ∼ 180 kV) place the electron source (cathode) and electron target (anode) in a
sealed glass tube. The anode and cathode extend from the glass tube, which acts as an insulator between these
electrodes. Further, the glass tube contains the necessary vacuum through which electrons are accelerated by
the applied high voltage between the anode and cathode. The anodes of x-ray tubes incorporate a suitable
metal upon which the electrons impinge and generate bremsstrahlung and characteristic x rays. Most of the
electron energy is deposited in the anode as heat rather than being radiated away as x rays and, thus, heat
removal is an important aspect in the design of x-ray tubes. Tungsten is the most commonly used target
material because of its high atomic number and because of its high melting point, high thermal conductivity,
and low vapor pressure. Occasionally, other target materials are used when different characteristic x-ray
energies are desired (see Table 5.5). Generally, the operating conditions of a particular tube (current,
voltage, and operating time) are limited by the rate at which heat can be removed from the anode. For most
medical and dental diagnostic units, voltages between 40 and 150 kV are used, while medical therapy units
may use 6 to 150 kV for superficial treatment or 180 kV to 50 MV for treatment requiring very penetrating
radiation.
Sec. 5.3. Sources of X Rays 167

Figure 5.3. Measured photon spectra from a Machlett Aeromax x-ray tube (tung-
sten anode) operated at a constant 140 kV potential. This tube has an inherent
filter thickness of 2.50-mm aluminum equivalent and yields the spectrum shown
by the thick line. The addition of an external 6-mm aluminum filter hardens the
spectrum (thin line). Both spectra are normalized to unit area. Data are from
Fewell, Shuping, and Hawkins [1981].

The energy spectrum of x-ray photons emitted from an x-ray tube has a continuous bremsstrahlung
component up to the maximum electron energy (i.e., the maximum voltage applied to the tube). If the
applied voltage is sufficiently high as to cause ionization in the target material, there will also be characteristic
x-ray lines superimposed on the continuous bremsstrahlung spectrum. In Fig. 5.3 two calculated exposure
spectra of x rays are shown for the same operating voltage but for different amounts of beam filtration (i.e.,
different amounts of material attenuation in the x-ray beam). As the beam filtration is increased, the low-
energy x rays are preferentially attenuated and the x-ray spectrum hardens and becomes more penetrating.
Also readily apparent in these spectra are the tungsten Kα1 and Kβ1 characteristic x rays.
The characteristic x rays may contribute a substantial fraction of the total x-ray emission. For example,
the L-shell radiation from a tungsten target is between 20% and 35% of the total energy emission when
voltages between 15 kV and 50 kV are used [ICRU 1970]. Above and below this voltage range, the L
component rapidly decreases in importance. However, even a small degree of filtering of the x-ray beam
effectively eliminates the low-energy portion of the spectrum containing the L-shell x rays. The higher-
energy K-series x rays from a tungsten target contribute a maximum of 12% of the total x-ray exposure for
operating voltages between 100 and 200 kV [ICRU 1970].
An ideal x-ray spectrum can be estimated from Eq. (5.7). The rate Ṅ (E) at which bremsstrahlung
energy, per unit energy about E, is produced in the target (MeV per second) when bombarded by a current
of I amperes of electrons which have been accelerated through a potential of V volts is
 
I  3 Eo
Ṅ (E) = ENbr (Eo , E)  Ik Eo − E − E ln , (5.11)
qe 4 E

in which qe is the electron charge, k  a constant, and Eo = 10−6 V . This spectrum, which is proportional to
the exposure spectrum, is an ideal thick target spectrum in that the incident electron is completely stopped
and no absorption of photons is considered. It is accepted practice in x-ray technology to use the dimensional
(not Compton) x-ray wavelength λ rather than the photon energy E. Since these two quantities are related
by λ = hc/E, the ideal spectral distribution of bremsstrahlung energy emission rate per unit wavelength,
168 Sources of Radiation Chap. 5

Ṅ (λ), is      
 dE   1 λ 3 λ

Ṅ (λ) = Ṅ (E)   = Ik 3 − 1 − ln , (5.12)
dλ  λ λo 4 λo
where the minimum wavelength λo = hc/Eo and k  is a constant. As the voltage increases above the critical
voltage for ionization of the target atoms, the emission rate of the characteristic x rays also increases. For
voltages up to six times the critical voltage for K-shell ionization, VK , the emission of the Kα x rays increases
approximately as (V − VK )2 [Flügge 1957].
The shape of the x-ray spectrum from a real x-ray machine, such as those of Fig. 5.3, differs considerably
from the ideal spectrum discussed above. The high-voltage power supply of most units usually does not
provide a constant voltage across the x-ray tube but rather gives a pulsating or fluctuating voltage.4 This
results in fewer high energy bremsstrahlung photons near the cutoff than would be expected on the basis of
the peak voltage alone. In effect, electrons with a distribution of energies up to the peak voltage impinge on
the anode and cause a shift of the bremsstrahlung spectrum toward lower energies (longer wavelengths). On
the other hand, the low-energy photons are preferentially absorbed by the target material, the glass envelope
of the x-ray tube, and the air outside the tube. In addition, metal filters are often placed in the beam path
to absorb preferentially the low-energy photons and thus to shift the spectrum toward higher energies. The
strength of the x-ray beam thus depends on the target material, tube voltage, tube current, and the type
and amount of filtering experienced by the x rays.

5.3.4 Synchrotron X Rays


When a charged particle initially moving in a straight line is accelerated by deflecting it in an electromagnetic
field, the perturbation in the particle’s electric field travels away from the particle at the speed of light and
is observed as electromagnetic radiation (photons). Such is the origin of bremsstrahlung produced when fast
electrons (beta particles) are deflected by the electric field of a nucleus.
This same mechanism can be used to produce intense photon radiation by deflecting an electron beam
by magnetic fields. In a special accelerator called a synchrotron, highly relativistic electrons are forced to
move in a circular path inside a storage ring by placing bending magnets along the ring. Photons are emitted
when the beam is accelerated transversely by (1) the bending magnets (used to form the circular electron
beam), and by (2) insertion device magnets such as undulators, wigglers, and wave-length shifters.
Because the electrons are highly relativistic, the synchrotron radiation is emitted in a very narrow cone in
the direction of electron travel as they are deflected. Undulators cause the beam to be deflected sinusoidally
by a weak oscillatory magnetic field, thereby producing nearly monochromatic photons. By contrast, a
wiggler uses a strong oscillatory magnetic field which, because of relativistic effects, produces distorted
sinusoidal deflections of the electron beam and synchrotron radiation with multiple harmonics, i.e., a line
spectrum. If very strong magnetic fields are used, many harmonics are produced that merge to yield a
continuous spectrum ranging from the infrared to hard x rays. By placing undulators or wigglers at a
specific location in the storage ring, very intense and narrowly collimated beams of photons with energies
up to a few keV can be produced, useful in x-ray diffraction analyses.

5.4 Sources of Neutrons


5.4.1 Fission Neutrons
Many heavy nuclides fission after the absorption of a neutron, and some nuclides fission spontaneously,
producing several energetic fission neutrons. Almost all of the fast neutrons produced from a fission event

4 If
a constant potential is applied to the x-ray tube, the designation “kVcp” is sometimes used, while the peak voltage for a
pulsating applied voltage is often indicated by “kVp.”
Sec. 5.4. Sources of Neutrons 169

Figure 5.4. Energy spectra of prompt neutrons produced from the


fission of fissionable nuclei as calculated by Walsh [1989].

are emitted within 10−14 s of the fission event, and are called prompt neutrons. Generally less than 1% of the
total fission neutrons are emitted as delayed neutrons, which are produced by the neutron decay of fission
products at times up to many seconds or even minutes after the fission event. As the energy of the neutron
which induces the fission in a heavy nucleus increases, the average number of fission neutrons also increases.
For example, the fission of 235 U by a thermal neutron (average energy 0.025 eV) produces, on the average,
2.43 fission neutrons. A fission caused by a 10-MeV neutron, by contrast, yields 3.8 fission neutrons. For
239
Pu, fission by thermal or 10 MeV neutrons yields 2.87 or 4.2 neutrons. The fission of 238 U is induced only
by fast neutrons, with a 10-MeV neutron yielding 3.9 fission neutrons.
Since the advent of fission reactors, many transuranic isotopes have been produced in significant quanti-
ties. Many of these isotopes have appreciable spontaneous fission probabilities, and consequently they can
be used as very compact sources of fission neutrons. For example, 1 g of 252 Cf releases 2.3 × 1012 neutrons
per second, and very intense neutron sources can be made from this isotope, limited in size only by the need
to remove the fission heat through the necessary encapsulation. Almost all spontaneously fissioning isotopes
decay much more frequently by α emission than by fission.
The energy dependence of the fission neutron spectrum has been investigated extensively, particularly for
the important isotope 235 U. All fissionable nuclides produce prompt-fission neutrons with energy frequency
distributions that go to zero at low and high energies (see Fig. 5.4), reaching a maximum at about 0.7 MeV,
and have an average energy of about 2 MeV. The fraction of prompt fission neutrons emitted per unit energy
about E, χ(E), can be described quite accurately by a Watt distribution

χ(E) = ae−E/b sinh cE, (5.13)

where the parameters a, b and c depend on the fissioning isotope (see Table 5.6). The fission-neutron
spectrum for thermal-neutron fission of 235 U is often used as an approximation for other fissioning isotopes.

5.4.2 Fusion Neutrons


Neutrons can be produced as products of nuclear reactions in which energetic charged particles hit target
atoms. Most such reactions require accelerators to produce the energetic charged particles and hence such
neutrons are to be encountered only near accelerator targets.
170 Sources of Radiation Chap. 5

Table 5.6. Parameters for the Watt approximation of Eq. (5.13).

Nuclide Type of Fission a b c


233 U thermal 0.6077 1.1080 1.2608
235 U thermal 0.5535 1.0347 1.6214
239 Pu thermal 0.5710 1.1593 1.2292
232 Th fast (2 MeV) 0.5601 0.9711 1.8262
238 U fast (2 MeV) 0.5759 1.0269 1.5776
252 Cf spontaneous 0.6400 1.1750 1.0401

One major exception to the insignificance of charged-particle-induced reactions are those in which light
elements fuse exoergically to yield a heavier nucleus and which are accompanied quite often by the release of
energetic neutrons. Neutron-producing fusion reactions of most interest in the development of thermonuclear
fusion power are
2
H + 2 H −→ 3
He (0.82 MeV) + 1 n (2.45 MeV)
2
H + 3 H −→ 4
He (3.5 MeV) + 1 n (14.1 MeV).

When these reactions are produced by accelerating one nuclide toward the other, the velocity of the center
of mass must first be added to the center-of-mass neutron velocity before determining the neutron energy
in the laboratory coordinate system. In most designs for fusion power, the velocity of the center of mass is
negligible, and the concern is with monoenergetic 2.45- or 14.1-MeV fusion neutrons. The 14.1-MeV fusion
neutrons are also produced copiously in a thermonuclear explosion.
A beam of relatively low energy deuterons (100 to 300 keV) incident on a deuterium or tritium target
can produce a significant number of thermonuclear neutrons. Thus, these D-D or D-T reactions are used in
relatively compact accelerators, called neutron generators, in which deuterium ions are accelerated through
a high voltage (100 to 300 kV) and allowed to fall on a thick deuterium- or tritium-bearing target. Typically
in such devices, a 1-mA beam current produces up to 109 14-MeV neutrons per second from a thick tritium
target.

5.4.3 Photoneutrons
A gamma photon with energy sufficiently large to overcome the neutron binding energy (about 7 MeV in most
nuclides) may cause a (γ, n) reaction. Very intense and energetic photoneutron production can be realized in
an electron accelerator where the bombardment of an appropriate target material with the energetic electrons
produces intense bremsstrahlung (see Section 5.3.2) with a distribution of energies up to that of the incident
electrons. The probability a photon will cause a (γ, n) reaction increases with the photon energy, reaching
a maximum over a broad energy range of approximately 20 to 23 MeV for light nuclei (A < ∼ 40) and 13 to
18 MeV for medium and heavy nuclei. The peak energy of this giant resonance can be approximated by
80A−1/3 MeV for A > 40. The width of the resonance varies from about 10 MeV for light nuclei to 3 MeV
for heavy nuclei. Consequently, in medical or accelerator facilities that produce photons with energies above
about 15 MeV, neutron production in the surrounding walls can lead to significant neutron fields.
The photoneutron mechanism can be used to create laboratory neutron sources by mixing intimately a
beryllium or deuterium compound with a radioisotope that decays with the emission of high energy photons.
Sec. 5.4. Sources of Neutrons 171

Alternatively, the encapsulated radioisotope may be surrounded by a beryllium- or deuterium-bearing shell.


A common reactor photoneutron source is an antimony-beryllium mixture, which has the advantage of being
rejuvenated by exposing the source to the neutrons in a nuclear reactor to transmute the stable 123 Sb into the
required 124 Sb isotope (half-life of 60.2 days). Characteristics of some (γ, n) sources are given in Table 5.7.
One very attractive feature of such (γ, n) sources is the nearly monoenergetic nature of the neutrons if
the photons are monoenergetic. However, in large sources, the neutrons may undergo significant scattering
in the source material and thereby degrade the nearly monoenergetic nature of their spectrum. These
photoneutron sources generally require careful use because of their inherently large photon emission rates.
Because nominally only one in a million high energy photons actually interacts with the source material to
produce a neutron, these sources generate gamma rays that are of far greater biological concern than are
the neutrons. A particularly useful combination is an SbBe neutron source coupled with an 56 Fe shield. The
56
Fe 24 keV anti-resonance allows the passage of the SbBe 23 keV neutrons while working to shield other
emissions.

Table 5.7. Characteristics of some important (γ, n) sources.

Average
Principal photons
neutron
Half- E Number energy Standard
Source
life (MeV) per decay (MeV) yielda
24 Na + Be 15.0 h 2.754 1.00 0.967 3.5
24 Na + D2 O 15.0 h 2.754 1.00 0.262 7.3
28 Al + Be 2.24 m 1.779 1.00 0.100
56 Mn + Be 2.58 h 1.810 0.272 0.128 0.78
2.113 0.143 0.397
2.522 0.010 0.761
56 Mn + D2 O 2.58 h 2.522 0.010 0.146 0.08
2.657 0.007 0.214
72 Ga + Be 14.1 h 1.861 0.053 0.173 1.4
2.202 0.259 0.476
2.491 0.077 0.733
2.508 0.128 0.748
72 Ga + D2 O 14.1 h 2.491 0.077 0.131 1.6
2.508 0.128 0.139
76 As + Be 26.3 h 1.788 0.003 0.108 1.9
2.096 0.007 0.382
88 Y + Be 107 d 1.836 0.993 0.151 2.7
2.734 0.006 0.949
88 Y + D2 O 107 d 2.734 0.006 0.252 0.08
116m In + Be 54.2 m 2.112 0.154 0.396 0.22
124 Sb + Be 60.2 d 1.691 0.490 0.023 5.1
2.091 0.057 0.378
140 La + Be 40.4 h 2.522 0.034 0.761 0.08
140 La + D2 O 40.4 h 2.522 0.034 0.146 0.2
226 Ra + Be 1622 y many 0.68 max 0.8
226 Ra + D O 1622 y many 0.11 max 0.03
2
228 Ra + Be 6.7 y 2.62 0.848 0.95
1.80 0.119
228 Ra + D2 O 6.7 y 2.62 0.195 2.6

a Number of neutrons emitted from 1 g of Be or D O per 106 disintegrations


2
of the radionuclide placed 1 cm away. Yield is for all photons emitted.
Sources: Blizard and Abbott [1962], Shleien [1992], and Shultis and Faw
[2000]
172 Sources of Radiation Chap. 5

5.4.4 Alpha-Neutron Sources


Many compact laboratory neutron sources use energetic alpha particles from various radioisotopes (emitters)
to induce (α, n) reactions in appropriate materials (converters). Although a large number of nuclides emit
neutrons if bombarded with alpha particles of sufficient energy, the energies of the alpha particles from
radioisotopes are capable of penetrating the potential barriers of only the lighter nuclei.
Of particular interest are those light isotopes for which the (α, n) reaction is exoergic (Q > 0) or, at least,
has a low threshold energy. For endoergic reactions (Q < 0), the threshold alpha energy is −Q(1 + 4/A).
Thus, for an (α, n) reaction to occur, the alpha particle must (1) have enough energy to overcome the repulsive
Coulombic force field of the nucleus, and (2) exceed the threshold energy for the reaction. Converter materials
used to make practical (α, n) sources include lithium, beryllium, boron, carbon, fluorine and sodium.
A neutron source can be fabricated by mixing intimately a light converter element, such as lithium or
beryllium, with a radioisotope that emits energetic alpha particles. Most of the practical alpha emitters
are actinide elements, which form intermetallic compounds with beryllium. Such a compound, e.g., PuBe13 ,
ensures both that the emitted alpha particles immediately encounter converter nuclei, thereby producing
a maximum neutron yield, and that the radioactive actinides are bound into the source material, thereby
reducing the risk of leakage of the alpha-emitting component.
The neutron yield from an (α, n) source varies strongly with the converter material, the energy of the
alpha particle, and the relative concentrations of the emitter and converter elements. The degree of mixing
between converter and emitter and the size, geometry, and source encapsulation may also affect the neutron
yield. For example, a 239 Pu/Be source has an optimum neutron yield of about 60 neutrons per 106 primary
alpha particles. Characteristics of some (α, n) sources are given in Table 5.8.

Table 5.8. Characteristics of some (α, n) sources.

Principal Average Optimum neutron


Half-
Source alpha energies neutron yield per 106
life
(MeV) energy (MeV) primary alphasa
210 Po / Li 138.4 d 5.305 0.48 1.3
239 Pu / Be 24100 y 5.155, 5.143, 5.105 4.6 60
210 Po / Be 138.4 d 5.305 4.5 70
238 Pu / Be 87.8 y 5.499, 5.457, 5.358 4.5 80
241 Am / Be 432 y 5.486, 5.443, 5.388 4.4 75
244 Cm / Be 18.1 y 5.805, 5.763 4.3 100b
242 Cm / Be 163 d 6.113, 6.070 4.1 110
226 Ra / Be 1600 y 7.687, 6.003, 5.490 3.9 500c
+ daughters 5.304, 4.785, 4.602
227 Ac / Be 21.8 y 7.386, 6.819, 6.623 3.9 700c
+ daughters 6.038, 5.960, 5.715
241 Am / B 432 y 5.486, 5.443, 5.388 3 13
210 Po / C 138.4 d 5.305 0.10
241 Am / F 432 y 5.486, 5.443, 5.388 1.5 4.1
210 Po / F 138.4 d 5.305 5
210 Po / Na 138.4 d 5.305 1
a Yield for alpha particles incident on a target thicker than the alpha-particle ranges.
b Does not include a 4% contribution from the spontaneous fission of 244 Cm.

c Yield is dependent on the proportion of daughters present. Value for 226 Ra corresponds
to a 22-year-old source (50% contribution for 210 Po).
Sources: Jaeger [1968], GPO [1970], and Knoll [1989].
Sec. 5.4. Sources of Neutrons 173

The energy distributions of neutrons emitted from (α, n) sources are continuous below some maximum
neutron energy with definite structure at well-defined energies determined by the energy levels of the converter
and the excited product nuclei (see Fig. 5.5). The use of the same converter material with different alpha
emitters produces similar neutron spectra with different portions of the same basic spectrum accentuated or
reduced as a result of the different alpha-particle energies. Average energies of neutrons typically are several
MeV. For example, the neutrons produced by a 239 Pu/Be source have an average energy of 4.6 MeV.

Figure 5.5. Neutron energy spectra produced by four (α, n) sources. The spectral structure
is determined by the converter material, while the relative intensity of various portions of the
spectrum depends on the energies of the alpha particles emitted by the radioactive component.
Based on experiment data from Anderson and Neff [1972] and Lorch [1973].

5.4.5 Activation Neutrons


A few highly unstable nuclides decay by the emission of a neutron. The delayed neutrons associated with
fission arise from such decay of the fission products. However, there are nuclides other than those in the
fission-product decay chain which also decay by neutron emission. Only one of these nuclides, 17 N, is of
importance in nuclear reactor situations. This isotope is produced in water-moderated reactors by an (n, p)
reaction with 17 O (threshold energy, 8.0 MeV). The decay of 17 N by beta emission (half-life 4.4 s) produces
17
O in a highly excited state, which in turn decays rapidly by neutron emission. Most of the decay neutrons
are emitted within ± 0.2 MeV of the most probable energy of about 1 MeV, although neutrons with energies
up to 2 MeV may be produced.

5.4.6 Spallation Neutron Sources


In a spallation neutron source, pulses of very energetic protons (up to 1 GeV), produced by an accelerator,
strike a heavy metal target such as mercury or liquid bismuth. Such an energetic proton when it strikes a
target nucleus “spalls” or knocks out neutrons. Additional neutrons boil off as the struck nucleus heats up.
Typically, 20 to 30 neutrons are produced per spallation reaction. These pulses of neutrons are then slowed
down or thermalized by passing them through cells filled with water, or even liquid hydrogen if very slow
neutrons are needed.
174 Sources of Radiation Chap. 5

5.5 Sources of Charged Particles


Charged particles are directly ionizing radiations and, unlike photons and neutrons, have well-defined ranges
as they interact with the long-range Coulombic forces of the atoms of the medium through which they
pass. Such particles arise from several sources. Radioactive decay products almost always produce charged
particles such as alpha and beta particles.5 Likewise, photon and neutron induced reactions with an atom
usually produce secondary charged particles. Indeed it is these secondary charged particles that are used to
detect the presence of these indirectly ionizing radiations. Finally in our technological modern world there are
many machines that produce energetic charged particles. Indeed accelerators that produce energetic charged
particles are used for a myriad of tasks such as industrial processing, production of medical radioisotopes,
or numerous research purposes.

5.5.1 Beta Decay


Beta decay of a radionuclide, in effect, involves either (1) a transformation within the nucleus of a neutron
into a proton accompanied by the emission of an electron, or beta particle, and an antineutrino, or (2)
a nuclear transformation of a proton in the decaying nucleus to a neutron accompanied by emission of a
positron and a neutrino. The energy released in the process—the Q value—is shared by the electron and
the antineutrino or by the positron and the neutrino. Beta decay of a nucleus may occur by any of several
different nuclear transitions. For each there is a unique endpoint energy, the maximum kinetic energy of the
electron or positron. Also, for each transition, there is a unique statistical distribution of energy between
the electron and antineutrino or positron and neutrino, and to a very minor extent the residual nucleus. The
balance of this discussion deals with the more common beta-particle emissions, with the recognition that
positron emission may be treated very similarly.
Although the energy spectrum of the beta particles
for any one transition certainly depends on the endpoint
ΔJ ΔΠ Transition classification n
energy, the spectrum also depends, in a complicated
0,1 −1 Allowed 0 way, on the nuclear spin and parity quantum numbers
0,1 +1 Non-unique, first-forbidden 0 of the nucleus before and after beta-particle emission.
2 +1 Unique, first-forbidden 1 As shown to the left, these quantum numbers deter-
2 −1 Non-unique, second-forbidden 1 mine whether the transition is referred to as allowed or
3 −1 Unique, second-forbidden 2 forbidden, and if forbidden, whether the transition is
unique (U) or non-unique (non-U). In a transition, the
spin quantum number J may remain constant or it may change by one or more units, that is, ΔJ = 0, 1, 2, . . . .
The parity quantum number Π may or may not change, that is, ΔΠ = −1 (no change) or +1 (change). To
a first approximation, a single classification index n may be used to characterize the energy spectrum. For
ΔJ ≥ 2, n = ΔJ − 1. Otherwise, the various combinations of ΔΠ and ΔJ establish the following selection
rules, which determine the shape factor, which, in part, governs the beta-particle energy spectrum for a
particular transition.
As an example, consider the decay of 38 Cl to 38 Ar. Three beta transitions are possible, with the following
characteristics:

5 Only in gamma-ray decay of nuclear isomers, electron capture, and neutron radioactive decay (from fission fragments, for
instance) are no charged particles emitted.
Sec. 5.5. Sources of Charged Particles 175

Frequency Emax Eav


(%) (keV) (keV) ΔJ ΔΠ n Classification
32.5 1107 420 1 −1 0 Allowed
11.5 2749 1182 0 +1 0 Non-U, first forbidden
56.0 4917 2244 2 +1 1 Unique, first forbidden

The energy spectrum of beta particles arising from a transition is conveniently expressed in terms of
the √electron total energy W (including rest-mass energy), that is, W = E + me c2 , and the momentum
p = E 2 + 2me c2 E/c . The energy spectrum Ni (E) for transition i is defined in such a way that Ni (E)dE
is the probability that, in a transformation of the radionuclide via transition i, a beta particle is emitted
with kinetic energy in the range dE about E. This spectrum can be expressed as

Ni (E) = Ci p W [Emax,i − E]2 F (Z, A, W ) Sn (Z, A, Emax,i , W ), (5.14)

in which Emax,i represents the maximum (or endpoint) energy, Z and A are the charge and mass numbers of
the nucleus after the transition, F is the Fermi function, Sn is a shape factor determined by the selection-rule
classification index n, and Ci is a normalization constant.

Figure 5.6. Energy spectra of 38 Cl beta Figure 5.7. Energy spectra of selected beta-
particles. particle sources.

The product p W [Emax,i − E]2 is a statistical factor and is a major determinant of the energy spectrum.
The shape factor Sn is unity for allowed and nonunique first-forbidden transitions; for other transitions it
is a complicated function. Suffice to say here that it is an extremely tedious task to evaluate the Fermi
function and the shape factor. Procedures are clearly described by Dillman and Von der Lage [1975] and
by Dillman [1980], as are procedures required to account for screening by atomic electrons, an effect that
is especially important for positron decay. Figure 5.6 illustrates individual and composite spectra for the
three transitions involved in the beta decay of 38 Cl. In Fig. 5.7 the spectra for four important beta-emitting
radionuclides are given. Table 5.9 lists commonly encountered radionuclide sources that emit beta particles.
If fi is the frequency for the ith transition, then the spectrum normalization constant Ci is determined
by the requirement that
 Emax,i
dE Ni (E) = fi . (5.15)
0
176 Sources of Radiation Chap. 5

Table 5.9. Half-lives of common beta-particle emitters, maximum


emission energies, and yields. Positron emission is indicated by (+).

Nuclide Half-life Emax (MeV) % yield


3H 12.26 y 0.0186 100
63 Ni 100.1 y 0.067 100
14 C 5730 y 0.156 100
35 S 87.51 d 0.167 100
147 Pm 2.6234 y 0.224 99.994
33 P 25.34 d 0.249 100
45 Ca 163.8 d 0.257 100
99 Tc 2.111×105 y 0.294 99.998
22 Na 2.602 y 0.545(+) 90.3
1821(+) .055
131 I 8.02 d 0.304 0.643
0.334 7.20
0.606 89.4
0.807 0.39
36 Cl 3.01×105 y 0.710 98.1
204 Tl 3.78 y 0.764 97.08
210 Pb/210 Bi 22.3 y/ 5.01 d 0.017 80.2
0.064 19.8
1.161 99.99
137 Cs 30.07 y 0.514 94.36
1.176 5.64
60 Co 5.271 y 0.317 99.88
1.491 0.12
32 Si/32 P 172 y/ 14.26 d 0.225 100
1.710 100
68 Ge/68 Ga 270.8 d/ 67.63 m 0.822(+) 1.2
1.899(+) 87.68
90 Sr/90 Y 28.78 y/ 64.1 hr 0.546 100
2.280 99.99
106 Ru/106 Rh 1.023 y/ 29.8 s 0.039 100
1.979 1.77
2.407 10.0
3.029 8.1
3.541 78.6

Sources: Firestone [1996]; NUDAT [2019].

The average beta-particle energy for a particular transition is


 Emax,i
1
Ei  = dE ENi (E). (5.16)
fi 0
%
The average beta-particle energy released per transformation of the radionuclide is given by i fi Ei .

5.5.2 Alpha Decay


Radioactive decay by alpha-particle emission is possible only in the heavier elements. One radionuclide
may have several transitions involving alpha-particle emission; but for each transition, the particles are
monoenergetic and usually of several MeV energy. The Geiger-Nuttall rule [Kaplan 1962] accounts for the
strong inverse relationship between the half-life of a radionuclide and the energy of its alpha particle. Table
5.10, which lists several important alpha-particle emitters, illustrates this inverse relationship.
Sec. 5.5. Sources of Charged Particles 177

Table 5.10. Half-lives of common alpha-particle emitters. Also


listed are the prominent energies and frequencies of particles emitted.

Nuclide Half-life E (MeV) Percent


252 Cf† 2.645 y 6.118 84.3
6.076 15.5
244 Cm 18.11 y 5.805 76.4
5.763 23.6
238 Pu 87.74 y 5.499 71.4
5.456 28.6
241 Am 432.2 y 5.486 85.1
5.443 12.8
5.388 1.4
228 Th 1.913 y 5.423 73.4
5.340 26.6
(228 Th has multiple daughters ranging from 5.449 to 8.784 MeV)
210 Po 138.4 d 5.304 100
239 Pu 2.411×104 y 5.157 73.3
5.144 15.1
5.106 11.5
226 Ra 1600 y 4.785 94.4
4.602 5.5
(226 Ra has multiple daughters ranging from 5.489 to 7.687 MeV)
237 Np 2.14×106 y 4.789 47.6
4.774 18.1
4.769 14.3
4.644 5.9
230 Th 7.538×104 y 4.687 76.3
4.621 23.4
235 U 7.038×108 y 4.596 5.6
4.398 57
4.366 17
4.214 6.4
238 U 4.468×109 y 4.198 77
4.151 23
232 Th 1.405×1010 y 4.013 77
3.950 23
148 Gd 74.6 y 3.183 100

Source: Firestone [1996].


† Also a spontaneous neutron emitter.

5.5.3 Photon Interactions


In all the principal photon interactions, secondary electrons are produced. The photoelectric interactions lead
to photoelectrons and, perhaps, Auger electrons. In a Compton scattering interaction, an orbital electron
recoils from the atom, and in pair production a positron-electron pair are created. The energetics of these
secondary electrons are discussed in Sections 4.3.3 and 4.4. X- and gamma-ray detectors then measure the
ionization and excitation of the ambient atoms produced by these secondary electrons.
178 Sources of Radiation Chap. 5

5.5.4 Neutron Interactions


Scattering
Often, when neutrons interact with a nucleus, secondary charged particles are produced. When fast neutrons
scatter from a nucleus, the recoil nucleus is a charged particle which gives up its kinetic energy through
ionization and excitation of the ambient atoms. The energy transfered from the neutrons to the recoil
nucleus is described in Section 4.3.4. As the mass of the scattering nucleus decreases ever more energy is
transferred to the recoil nucleus. In particular, for scattering from hydrogen, the recoil nucleus (a proton)
can receive up to all of the incident neutron’s energy. By measuring the energy distribution of the recoil
protons, the energy distribution of the fast incident neutrons can be inferred.
Because the neutron has an internal charge distribution that is not uniform throughout the neutron, it is
possible for neutrons to interact with electrons. However, such neutron-electron interactions are exceedingly
rare and are of little importance in radiation detection.
Charged-Particle Reactions
Neutron detectors are often designed to detect the charged particles produced in neutron reactions that
produce secondary charged particles. Most such reactions such as 3 He(n, p)3 H, 10 B(n, α)7 Li, or 6 Li(n, t)4 He,
occur predominately at thermal neutron energies. However, for neutrons with energies in the MeV region
(n, p), (n, α) and other knockout reactions can also occur. These reactions are especially important when
light elements are involved. The (n, α) reaction cross sections for Be, N, and O are appreciable fractions
of the total cross sections and may exceed the inelastic scattering contributions. This situation is probably
true for most light elements, although only partial data are available. For heavy and intermediate nuclei,
the charged-particle emission interactions are at most a few percent of the total inelastic interaction cross
sections and, hence, are usually ignored.
Fission
A special case of charged-particle producing reactions is that of neutron-induced fission. Any very heavy
nucleus can be made to fission accompanied by a net release of energy if hit sufficiently hard by some incident
particle. However, very few nuclides can fission by the absorption of a neutron with negligible incident
kinetic energy. The binding energy of this neutron in the com-
pound nucleus provides sufficient excitation energy that the com-
pound nucleus can deform sufficiently to split spontaneously. Nu-
clides, such as 235 U, 233 U, and 239 Pu, that fission upon the ab-
sorption of a slow moving neutron, are called fissile nuclei and
play an important role in thermal neutron fission detectors. Nu-
clides that fission only when struck with a neutron with one or
more MeV of kinetic energy, such as 238 U and 240 Pu, are said to
be fissionable, i.e., they undergo fast fission.
The highly excited compound nucleus almost always splits
assymetrically producing a heavy fission fragment YH and a
lighter fission fragment YL .6 The initial fission fragments are
highly charged, missing 10 to 15 electrons. They are also in such
highly excited states that, within 10−17 s of the scission, several Figure 5.8. Energy distribution of fission prod-
235
prompt neutrons “boil” away, and, within 2×10−14 s, more exci- ucts produced by the thermal fission of U. The
mean energy of the light fragment is 99.2 MeV
tation energy is lost from the emission of prompt fission gamma and that of the heavy fragment is 68.1 MeV. Af-
rays. ter Keepin [1965].

6 Sometimes three fission fragments are formed in ternary fission with the third being a small nucleus. Alpha particles are
created in about 0.2% of the fissions and nuclei of 2 H, 3 H, and other nuclei up to about 10 B with much less frequency.
Sec. 5.6. Cosmic Rays 179

The highly charged fission fragments pass through the surrounding medium causing millions of Coulombic
ionization and excitation interactions with the electrons of the medium. As the fission fragments slow, they
gradually acquire electrons that reduce their ionization charge, until, by the time they are stopped, they
have become electrically neutral atoms. This transfer of the fission fragments’ kinetic energy to the ambient
medium takes about 10−12 s. It is this enormous energy transfer to the ambient medium that makes neutron
fission detectors possible.
Because the mass distribution of the fission fragments is bimodal (two peaks), one would expect the
initial kinetic energy of the fragments to also be bimodal. In Fig. 5.8, the kinetic energy distribution of the
fission fragments produced in the thermal fission of 235 U is shown.

5.5.5 Accelerators
Beginning in the 1930s, machines were developed to accelerate charged subatomic particles such as protons
and alpha particles to speeds that could induce nuclear reactions. The first such particle accelerator produced
protons with 700 keV of energy. Recently an accelerator became operational that produces 7-TeV protons
or heavy ions such as lead with 1200 TeV of kinetic energy.
Today the development of ever more energetic particle accelerators is driven by the high energy physics
community. With these enormous and costly machines, physicists will perform experiments that will reveal
information about the fundamental physics governing the subatomic world. Accelerators with lower energies
are also central to other areas of research such as the study of atomic and nuclear physics. A 1-GeV
proton accelerator is now used at the Spallation Neutron Source at Oak Ridge National Laboratory to
bombard a liquid mercury target. The resulting spallation reactions release copious neutrons which are
ideal probes to determine molecular structures. Accelerators can also be used to produce intense x-ray
beams that in turn can be used in fundamental research on materials. As in most areas of fundamental
research, accelerator technology has spun off many practical applications such as cancer therapy, production
of important radionuclides, ion implanting, and food preservation to name a few.
For high energy physics research, special radiation detectors are needed to detect the myriad of subatomic
particles that are produced in these machines. Such detectors are huge, very expensive, and usually one of
a kind. Consequently, only brief consideration of such detectors is given in this book.

5.6 Cosmic Rays


At the beginning of the twentieth century, the reason why electrometers would discharge for no apparent
reason was a mystery. One postulated explanation was that earth itself emitted ubiquitous ionizing radiation.
But in 1911 Victor Hess, using electrometers on a balloon, found that ionizing radiation increased in strength
with altitude, thereby showing that this radiation came from outer space.
Although much is now known about this cosmic radiation, there are many aspects of it that are still
mysterious. Cosmic radiation has been measured from a few GeV to over 1020 eV. At a few GeVs the
composition is 98% nuclei (of which 87% are protons, 12% helium nuclei, and 1% heavier nuclei), < 2%
electrons, and < 10−4 % gamma rays. One unsettled question is how the most energetic cosmic rays are
produced. For example, since 1991 more that 20 protons with energies ≥ 3 × 1020 eV have been observed.
This energy corresponds to 48 J, which is the kinetic energy of a 58-g tennis ball moving at about 150 km/h!
The energy spectrum of cosmic rays follows a “power law” E −α where α  2.7 for 1010 < E < 3 × 1015 eV
and, above 3 × 1015 eV, α  3.
At times, some stars throw off their outer sheath, forming a shock wave rapidly moving outward. In 1949
Enrico Fermi suggested that charged particles moving back and forth through a moving and magnetized
shock front would statistically gain energy. As a particle gains energy, the shorter is the time that the
180 Sources of Radiation Chap. 5

charged particle stays in the front of the shock wave, and the higher the probability it will escape. In such
a case, the charged particles leaving the front would have a power-law distribution in energies.
But where are such cosmic accelerators located? Prime suspects are Active Galactic Nuclei (AGN),
which are galaxies that produce more electromagnetic emission than can be deduced from their stellar
content, stellar remnants, and their interstellar medium. Such AGNs are assumed to harbor at their centers
a supermassive black hole, millions to billions more massive that our sun. Such a black hole accretes matter
from the surrounding galaxy, forming an accretion disk and two “jets,” each up to several thousand light-
years in length, perpendicular to the disk. In these jets it is thought that charged particles can be accelerated
to the highest possible energies and, in the process, more radiation is produced than by the entire galaxy.
Another possible source is a supernova remnant. The ejected outer shell of the supernova builds into a
spherically shaped nebula (the supernova remnant). The inner core of the supernova becomes a black hole,
a neutron star, or a white dwarf, depending on the mass of the progenitor star. A shock front is formed
when the ejected material flows into the interstellar medium. And in this shock front, Fermi acceleration
can occur that produces enormous numbers of relativistic particles.
A neutron star produced by a supernova explosion that spins with a period of less than a few seconds
is called a pulsar. Because pulsars have very strong corotating magnetic fields (> 1012 G), a strong electric
field is induced, which in turns accelerates charged particles.
Finally, microquasars, are binary systems consisting of a compact neutron star or black hole and a massive
companion star. The compact object accretes matter from the star forming an accretion disk that produces
a pair of perpendicular relativistic jets in which charged particles are accelerated, as occurs in AGNs.

5.6.1 High Energy Gamma Rays


Another cosmic ray mystery is how cosmic gamma rays with energies above several MeV are produced, the
so-called high energy (HE) and very high energy (VHE) gamma rays. The hottest structures in the universe
are accretion disks around compact objects. Yet their thermal peak emissions produce x rays with energies
up to only a few tens of keVs. Moreover, the energy spectrum of HE and VHE gamma rays is found to follow
a power law E −α , a distribution not followed by the thermal black body spectrum. Hence, high energy
gamma photons cannot be produced by thermal emissions.
The HE and VHE gamma rays undoubtedly arise because of the interaction of high energy charged
particles with matter. If a cosmic proton accelerator is surrounded by dense matter, copious numbers of
neutral pions π 0 are produced by the highest energy protons. The main decay mode of these pions (98.8%)
is into two very energetic gamma photons. Another mechanism involves relativistic electrons. In strong
magnetic fields these electrons lose energy through synchrotron and curvature emissions. Alternatively, in
inverse Compton scattering, a low energy photon scatters from a high energy electron to produce a high
energy photon.
Beginning in the 1960s it was revealed that bursts of gamma rays appeared randomly in the sky. Today it
is known that these gamma ray bursts (GRB) occur about once a day lasting from milliseconds to hundreds
of seconds and originate far outside our galaxy. The energy release is enormous and the mechanism(s) for
the creation of such bursts is not well established. Conjectured possibilities include the merging of two black
holes or two neutron stars and the collapse of a hypernova.
Problems 181

PROBLEMS
1. The average mass of potassium in the adult human body is about 140 g of which 0.0117% of the
radioisotope 40 K. (a) Estimate the average activity (Bq) of 40 K in the body. (b) From the data in
Ap. C, estimate the energy and number of gamma photons emitted per second from the body.
2. An obsolete unit of activity, although still widely used, is the curie (Ci) which equals 3.7 × 1010 Bq.
How many atoms and what mass of the isotope 3 H are needed to produce a radioactive source with an
activity of 1 Ci? Perform the same calculation for the isotopes 60 Co and 239 U.
14
3. Why does coal contain no C?

4. How many alpha particles are emitted per second from a 1-gram sample of vanadium? Compare this
emission rate to that for one gram of 238 U.

5. A 1-g sample of 235 U is placed in a thermal flux of 4 × 104 cm−2 s−1 . How many prompt fission gamma
photons are emitted per second from this sample?

6. The global inventory of 14 C is about 8.5 EBq. If all that inventory is a result of cosmic ray interactions
in the atmosphere, how many kilograms of 14 C are produced each year in the atmosphere?

7. Calculate the neutron emission rate from a 20-GBq point source of 124 Sb surrounded by 40 g of beryllium.
The 9 Be(γ, n) cross section is about 1 mb.

8. An isotope that decays by ejecting alpha particles with energies 6.82 MeV (10%) and 4.30 MeV (90%) is
mixed intimately with a large amount of beryllium. For an (α, n) source using 40 GBq of this mixture,
estimate the neutron emission rate and sketch the energy spectrum of the emitted neutrons.

9. Estimate the rate at which activation product neutrons from the decay of 17 N are produced in a water-
moderated, uranium-fueled reactor which is operating at a steady thermal power of 3000 MW.
238
10. Estimate the number of spontaneous-fission neutrons emitted from a 1 kilogram sample of U.

11. A thermonuclear device (2 H-3 H reaction only) is detonated in space with a yield of 1.00 MWd. What
is the resulting neutron fluence 1 km from the detonation point?

12. One gram of natural iron is present in a uniform thermal flux density of 1012 cm−2 s−1 . Describe
quantitatively the resulting emission of capture gamma rays from the iron.

13. A beam of thermal neutrons (1010 neutrons cm−2 s−1 ) irradiates a 2-g sample of calcium for 30 s. What
is the flux density (in vacuum) of gamma photons with energies greater than 1 MeV at a point 1 m
from the sample 2 min after the irradiation ceases? Consider the decay of both 47 Ca and 49 Ca.

14. Cadmium is commonly used to attenuate thermal neutrons because of its large (n, γ) cross section.
However, capture gamma photons are produced as a result of the neutron capture. As an example, use
Table B.4 to sketch the energy-dependent flux density of capture photons above 1 MeV at 10 m (in
vacuum) from a point where a thermal neutron beam of 108 neutrons s−1 is stopped by a cadmium
sheet.

15. Electrons accelerated through a potential of 100 kV strike a gold target. Sketch the spectrum of the
resulting x rays, first as a function of x-ray energy down to 50 keV, and, then as a function of wavelength.
Show both the bremsstrahlung and characteristic x rays. If the electron beam current and voltage were
182 Sources of Radiation Chap. 5

doubled and the target replaced by an aluminum one, by what percentage would the bremsstrahlung
power change?

16. Calculate the flux-density energy spectrum of the bremsstrahlung at 1 m (in vacuum) from a small
tungsten target bombarded by 10 mA of electrons accelerated through a constant potential of 500 kV.
Neglect x-ray absorption and assume isotropic emission of the x rays.

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99, 231–235, (1972). sion on Radiation Units and Measurements, 1970.
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topes, New York: Wiley, 1986.
KAPLAN, I., Nuclear Physics, 2nd Ed., Reading: Addison-Wesley,
DILLMAN,L.T., AND F.C. VON DER LAGE, Radionuclide Decay 1962.
Schemes and Nuclear Parameters for Use in Radiation Dose
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Medicine, 1975. Addison-Wesley, 1965.
DILLMAN, L.T., EDISTR—A Computer Program to Obtain a Nu- KNOLL, G.F., Radiation Detection and Measurement, 2nd Ed.,
clear Data Base for Nuclear Dosimetry, Report ORNL/TM- New York: Wiley, 1989.
6689, Oak Ridge, TN: Oak Ridge National Laboratory, 1980.
LORCH, E.A., “Neutron Spectra of 241 Am/B, 241 Am/Be,
ECKERMAN, K.F., R.J. WESTFALL, J.C. RYMAN, AND M. CRISTY, 241
Am/F, 242 Cm/Be, 238 Pu/13 C, and 252 Cf Isotopic Neutron
“Availability of Nuclear Decay Data in Electronic Form, Includ- Source,” Int. J. Appl. Radiat. Isot., 24, 585–591, (1973).
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338–345, (1994). [Available as DLC-172, NUCDECAY Data Li- NCRP, Radiation Protection Design Guidelines for 0.1–100 MeV
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1955; republished by Melbourne, FL: Krieger Publishing Co., www.nndc.bnl.gov/ nudat2/, accessed 2019.
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FAW, R.E., AND J.K. SHULTIS, “Radiation Sources,” Ch. 13, in RÉVAY, Z., R.B. FIRESTONE, T. BELGYA, AND G.L. MOLNÁR,
Encyclopedia of Sustainability Science and Technology, R.A. “Prompt Gamma-Ray Spectrum Catalogue,” in Handbook of
Meyers Ed., New York: Springer, ISBN 987-0-387-89469-0, pp Prompt Gamma Ray Activation Analysis in Neutron Beams,
343–387, 2012, . G. MOLNÁR, Ed. Dordrecht, The Netherlands: Kluwer Acad.
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Rockville, MD: U.S. Department of Health and Human Services, book, Silver Springs, MD: Scinta Inc., 1992.
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FIRESTONE, R.B., Table of Isotopes, 8th Ed. V.S. SHIRLEY, Ed. Park, IL: American Nuclear Society, 2000.
New York: Wiley, 1996.
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Pergamon Press, 1983.
Chapter 6

Probability and Statistics


for Radiation Counting

To understand God’s thoughts we must study statistics,


for these are the measure of His purpose.
Florence Nightingale1

6.1 Introduction
The science of probability can be traced to 1654 with a study of gambling, in which Blaise Pascal and
Pierre de Fermat were challenged with a die rolling problem. It was Chevalier de Méré who approached
Pascal and asked what the remaining chance of winning a game of dice would be between two players at
any moment during the progression of the game, with the idea that the two players would split the stakes
fairly if they wished to discontinue playing. The correspondence between Pascal and Fermat and their
early observations on probability and expected values have developed over time into a valuable science used
to interpret data and predict scientific outcomes. Although there are numerous definitions for statistics,
an accepted definition is that statistics is the branch of mathematics dealing with the collection, analysis,
interpretation, and presentation of numerical data. Presently, the fields of probability and statistics are
combined, in which collections of observed data are described by probabilistic models, making possible
predictions and categorization of observed phenomena.
The proper analysis of any type of experimental data requires an assessment of the uncertainties associated
with each measurement. Without such an estimate, the data have limited value. There are several types
of uncertainties or errors associated with any experimental measurement. These errors include stochastic
uncertainties, sampling errors and systematic errors. For example, the decay of radioactive atoms occurs
randomly or stochastically so that a measurement of the number of decays observed in a fixed time interval has
an inherent stochastic uncertainty. Repeated measurements would give slightly different results. Systematic
errors are introduced by some constant bias or error in the measuring system and are often very difficult to
assess because they may arise from biases unknown to the experimenter. Sampling errors arise from making
measurements on a different population from the one desired. These latter two errors are often hard to
detect, let alone quantify.
Engineers and scientists must always be aware of the difference between accuracy and precision, even
though popular usage often blurs or ignores the important distinction. Precision refers to the degree of

1 Lesserknown are Florence Nightingale’s contributions to the discipline of statistics. She collected much data on hospital
conditions and correlated her findings with death rates. She presented these results with her invention of statistical coxcomb
graphics, emphasizing the need for cleanliness in hospitals, ultimately leading to reformed hospital practices.

183
184 Probability and Statistics for Radiation Counting Chap. 6

measurement quantification as determined, for example, by the number of significant figures. Accuracy is a
measure of how closely the measured value is to the true (and usually unknown) value. A precise measurement
may also be very inaccurate. In radiation counting, methods of probability and statistics are used to provide
accurate measurements together with an estimate of the precision of the measurement, often termed the
error or uncertainty associated with the measurement. In this chapter, the fundamental probability and
statistical concepts used for radiation counting are introduced, along with associated probability models and
error analyses.

6.1.1 Types of Measurement Uncertainties


Data measured with an ionizing-radiation detection system contain both random uncertainties and systematic
errors. Uncertainty assignment requires knowledge of both. Even with a perfect measurement system
capable of operating over a long time period without introducing significant systematic error, one must
always consider the random nature of the data caused by the stochastic nature of all radiation sources. This
chapter deals only with one component of the total uncertainty—the random or statistical uncertainty, which
can be estimated through various probability distribution functions (PDFs), most commonly the Gaussian
(or normal) distribution.
Radiation counting is a stochastic process. Further complications in the data analysis can be introduced
if the source emission rate changes in time. For example, the activity of a single radionuclide sample
exponentially decays in time or the radiation leaking from a reactor increases in time as the reactor power
increases. In this chapter, unless otherwise noted, it is assumed that the strength of any radiation source is
constant in time.

6.1.2 Probability and Statistics


The term probability refers to the study of randomness and uncertainty in a series of non-deterministic
or stochastic measurements, and naturally arises from the study of an expected value of certain possible
outcomes as compared to all possible outcomes. One common example would be the toss of a fair coin,
where it is assumed that one side or the other (heads or tails) lands horizontally up when the tossed coin
comes to rest. Suppose that heads is selected as a “success” should it land face up. Because there are only two
possible outcomes from a coin toss and only one method by which a heads can be observed, the probability
is equal to the one possible method of observing a heads divided by two possible outcomes, or 1/2. Another
example is that of rolling a six-sided die, and each side of the die has a different number ranging from one
to six. Suppose that rolling a number one is considered a “success”. There are six possible outcomes, of
which only one outcome results in the observation of the number one. The anticipated outcome is divided
by the total number of possible outcomes to determine that there is a 1/6 probability of observing a number
one after one roll of the die. Chances are that the reader is already familiar with these examples, and the
results are intuitive. Yet, what of large sample sets, as expected with the observation of radioactive decay in
radioactive materials? Most materials have atomic densities between 1021 cm−3 and 1023 cm−3 ; hence even
tiny radioactive samples have enormous numbers of atoms which may decay within a certain time period
(or may not). For radioactive materials, how is the probability of observing an average number of radiation
emissions within a set time period predicted, and how is the uncertainty for experimental observations
determined and reported? To understand the models and methods used to predict, report, and analyze
radiation counting data, it is important to first define certain terms and statistical distributions commonly
used in probability theory and statistics.
Sec. 6.2. Probability and Cumulative Distribution Functions 185

6.2 Probability and Cumulative Distribution Functions


6.2.1 Continuous Random Variable
The probability distribution function (PDF) describes the expected outcomes for a random variable x over
the entire range of possible outcomes. A proper PDF has the following three properties: (1) it is defined
on an interval [a, b], where a < b, (2) it is non-negative on this interval although it can be zero for some
b
x ∈ [a, b], and (3) the PDF must be normalized such that a f (x) dx = 1. Here a and b represent real number
or infinite limits (i.e., a → −∞ and/or b → ∞) and the interval can be either closed or open.
A PDF is a density function, i.e., it specifies the probability per unit of x, so f (x) has units that are the
inverse of the units of x. The probability that x falls within the interval a ≤ x1 < x < x2 ≤ b is
 x2
Prob{x1 ≤ x ≤ x2 } = f (x) dx. (6.1)
x1

The integral defined by


 x
F (x) ≡ f (x ) dx , (6.2)
a

where f (x) is a PDF over the interval [a, b], is called the cumulative distribution function (CDF) of f . Note
that, from this definition, a CDF has the following properties: (1) F (a) = 0, (2) F (b) = 1, and (3) F (x) is
monotone increasing, because f is always non-negative.
The CDF is a direct measure of probability. The value F (xi ) represents the probability that a random
sample of the stochastic variable x has a value between a and xi , i.e., Prob{a ≤ x ≤ xi } = F (xi ). More
generally,  x2
Prob{x1 ≤ x ≤ x2 } = f (x) dx = F (x2 ) − F (x1 ). (6.3)
x1

6.2.2 Discrete Random Variable


Some PDFs are defined only for discrete values of a random variable x. For example, in rolling a die the
number of dots on the upward face has only six possible outcomes, namely x1 = 1, x2 = 2, . . . , x6 = 6. In
such cases, fi ≡ f (xi ) represents the probability of event i, where i = 1, 2, . . . , I. In general, the number of
outcomes I can be finite or unbounded. Then for f1 , f2 , . . . , fI to be a PDF it is required that (1) fi ≥ 0
%I
and (2) i=1 fi = 1. Further, the discrete CDF


i
Fi ≡ fj (6.4)
j=1

can be interpreted as the probability that one of the first i events occurs. This discrete CDF has the
properties that (1) F1 = f1 , (2) FI = 1, and (3) Fi ≥ Fj , if i ≥ j.

6.3 Mode, Mean and Median


Radiation measurements may consist of a single measurement or a series of measurements of a radioactive
source. Consider a set of measurements x1 , x2 , . . . , xN , where each xi is an observed value and N represents
the number of measurements taken. How are certain properties of this set of data determined, and which
properties contain important information to the experimenter? One such property may be a central value
of the data set, referred to as a location index [Kendall and Stuart 1977]. The location index may be the
186 Probability and Statistics for Radiation Counting Chap. 6

true value or an experimentally determined value. Further, the location index may be the mode (or most
probable value), the average (or mean value), or it may be the median (or middle) value of the data set. An
example of these three location indices is shown in Fig. 6.1.


  





 




     

Figure 6.1. Three often quoted location indices of a distribution
function, the mode xm , the median x̃, and the mean x.

6.3.1 Mode
The mode of a numerical data set is the most probable value, or the most frequently observed value, of that
data set. For a continuous function f (x) the mode is the value xm at which f (x) is maximum and is found
from 
df (x) 
 = 0. (6.5)
dx 
x=xm
For a discrete data set, the mode can be determined by noting the frequency at which a result is observed,
and selecting the most commonly observed result.
Unfortunately, f (x) may actually have several points that yield maxima in the distribution, hence the
mode may not be a unique attribute. For such a case, the PDF is said to be multimodal and each maximum
can be called a mode. However, in this book, the distribution functions that describe radiation counting
always have a single mode.

6.3.2 Mean
The mean of some random variable x, also referred to as the average or expected value of x, is defined for
any continuous function g(x) defined on the interval [a, b] as
 b & b
μ(x) ≡ xg(x) dx g(x) dx. (6.6)
a a
b
If g(x) is also a PDF, now represented by f (x), then a f (x) dx = 1 and the mean for a continuous PDF is
given by
 b
μ(x) = xf (x) dx. (6.7)
a
Sec. 6.4. Variance and Standard Deviation of a PDF 187

The mean of a PDF is sometimes denoted by x or by E(x) (for the expected value of x). More generally,
the central moments of a PDF are defined as
 ∞
n
μ(x ) = xn f (x) dx, n = 1, 2, . . . . (6.8)
−∞

Thus, the mean of a PDF is just the first central moment. The higher central moments give information
about the shape of the PDF. In fact, a PDF can be uniquely expressed in terms of its moments so that
knowing all the moments is tantamount to knowing the PDF itself [Cramèr 1946]. For a discrete PDF, the
mean is calculated as
1
I
μ(x) = xi fi . (6.9)
I i=1

6.3.3 Median
The median and mean of a variable are not the same, yet are often erroneously used synonymously as the
average. The word median actually refers to “middle,” not average. For a PDF the median x̃ or med(x) is
that value of x for which half the area under the distribution lies to the left of x̃ and half to the right of x̃,
i.e.,
 x̃  ∞
1
f (x) dx = f (x) dx = , (6.10)
−∞ x̃ 2
or, in words, the probability that x < x̃ is exactly equal to the probability that x > x̃.
To find the median of a discrete PDF, the fi are rearranged in ascending (or descending) order, from
smallest to the largest (or largest to smallest). The ordered sequence is denoted by f(1) , f(2) , . . . , f(I) . The
median is then defined as
$
middle value of f(i) , if I is odd
x̃ = . (6.11)
mean value of two middle f(i) ’s, if I is even

6.4 Variance and Standard Deviation of a PDF


As discussed above, PDFs have three location indices that give a measure of where the central portion of the
PDF is located, with the mean value x the most commonly used. However, this value gives no information
about the spread of the PDF for values above and below x. Typically, a location index, such as x, is quoted
along with a dispersion index, where the dispersion index is a measure of the spread of data relative to the
mean. From the definition of the mean one has for any PDF
 b 
I
(x − x)f (x)dx = 0 or (fi − μ(x)) = 0. (6.12)
a i=1

This result says that the average deviation from the mean is always equal to 0, and does little to assist with
a description of the spread of the PDF. Instead, the two most used dispersion indices in radiation counting
statistics are the variance and the standard deviation.
The variance for a continuous PDF f (x) is defined as
 b
σ 2 (x) ≡ var(x) = (x − μ(x))2 f (x)dx, (6.13)
a
188 Probability and Statistics for Radiation Counting Chap. 6

where σ(x) is the standard deviation (or standard error) of the PDF f (x) and μ(x) is the mean of the PDF
given by Eq. (6.7). From Eq. (6.13) the variance is seen to be the average value of (x − μ(x))2 and the
standard deviation is the positive root of that average value. Equation (6.13) can be rearranged as
 b  b  b  b
2
σ (x) = (x − μ(x)) f (x) dx =
2
x f (x)dx − 2μ(x)
2 2
xf (x) dx + μ (x) f (x) dx
a a a a

= μ(x2 ) − 2μ(x) μ(x) + μ2 (x) = μ(x2 ) − μ2 (x). (6.14)

Thus, the variance is the difference between the second central moment and the square of the first central
moment of the PDF. This  result is a far more meaningful and useful result compared to Eq. (6.13). The
standard deviation σ(x) = σ 2 (x) relates the spread about the mean value of a distribution function, and
hence allows an experimenter to quickly assess the expected error when designing an experiment that closely
follows a known PDF. For a discrete PDF a similar result is obtained for the variance:

I
σ 2 (x) ≡ (xi − μ)2 fi = μ(x2 ) − μ2 (x). (6.15)
i=1

6.5 Probability Data Distribution


Closely related to a discrete PDF is the data distribution function fD (xi ), which is an experimentally deter-
mined distribution function as distinct from a theoretical model. The data distribution function is defined
by a set of observed data. Suppose an outcome x is observed on occasion from a set of N trial experiments.
Typically, the number of times ni the desired outcome xi is observed is divided by the number of trials
conducted N . The only exact method to determine the probability f (xi ) of observing the outcome xi is to
perform an infinite number of trials, namely
ni
f (xi ) = lim . (6.16)
N →∞ N
Conducting an infinite number of trials is obviously impractical. In reality, an experimenter must decide
upon some practical finite number of N trials that can produce an estimate of p(xi ), within some acceptable
margin of error, as
ni
f (xi )  fD (xi ) = . (6.17)
N
In general, accuracy increases for the estimate of f (xi ) given by Eq. (6.17) as the number of trials N
increases. However, in some cases, an experimenter may be unable to perform a desired number of trials,
because, for example, of time constraints, and consequently must instead rely upon a smaller number of
trials. In such a case reporting the uncertainty associated with the estimated value of fD (xi ) is imperative.
As an example of constructing a data PDF, consider an experiment in which a radiation detector is used
to obtain a series Ĉ1 , Ĉ2 , . . . , ĈN of N measurements or counts (each under identical conditions).2 In this
set of N measurements, the number of resulting counts for some measurements may be equal; others may
be unique. The number of times ni identical counts xi are observed is tallied. This tallying % leads to a tally
sequence n1 , n2 , . . . , nM of observation of counts x1 , x2 , . . . , xM , where M (N ) ≤ N . Note Mi=1 n1 equals
the total number N of measurements made. The data distribution function is then determined by dividing
each tally by N , i.e.,

2 Throughout the text, a measurement is defined as the process of collecting counting data from a radiation detector, and a
count is defined as the single observation of a radiation event during a measurement.
Sec. 6.5. Probability Data Distribution 189

ni
fD (xi ) ≡ fDi = , i = 0, 1, 2, . . . , M. (6.18)
N
Here fDi is the estimate of the true probability f (xi ) of observing xi . Summation of all these estimates gives


M
n0 n1 n2 nM
fD (xi ) = + + + ... + = 1. (6.19)
i=0
N N N N

This result shows that a proper data PDF must be normalized to unity.

Example 6.1: Suppose the number of washing loads brought into a laundromat per person between the
hours of 1:00 pm and 4:00 pm one day are observed to be 1, 2, 1, 3, 2, 2, 3, 1, 4, 2, 1, 2. What is the data
distribution function?

Solution:
From the 12 persons observed, 4 people had 1 load, 5 people had 2 loads, 2 people had 3 loads, and only
1 person had 4 loads. Values for the data distribution function are as follows:
n1 4 n2 5
fD1 = = fD2 = =
12 12 12 12
n3 2 n4 1
fD3 = = fD4 = =
12 12 12 12
and fDn = 0 for n = 0 and n ≥ 5. By summing all possibilities, the data distribution function is shown to
be normalized, i.e.,
∞
4 5 2 1
fD (xi ) = 0 + + + + + 0 + 0 + ... = 1. (6.20)
i=0
12 12 12 12

6.5.1 Sample Mean


In most experiments, counts are accumulated and an average value is determined from the observations C i .
Hence, the data generally are in the form of discrete observations rather than as a continuous function. The
true mean of an experimentally observed random variable is correctly written as


I
1 
N 
M(N )
μ(x) = xi fi = lim Ci = lim xi fDi , (6.21)
N →∞ N N →∞
i=1 i=1 i=1

where as N → ∞ then M (N ) → I, the number of possible different observations. The above result indicates
that the exact value of an average can be determined only if an infinite number of measurements are recorded.
The luxury of conducting infinite measurements for an experiment is rare, hence a more practical method of
estimating the mean is to use an arithmetic average. This estimate is called the sample mean. The sample
mean (or experimental mean) is

1 
N
μ(x)  x = Ci . (6.22)
N i=1
190 Probability and Statistics for Radiation Counting Chap. 6

It should be remembered that the sample mean is only an approximation or estimate of the true mean, As
more measurements are made, thereby increasing N , it is expected that the value x approaches the true mean
μ(x). Usually, x is believed to yield a more accurate result of the expected value if a series of measurements is
made rather than any single measurement, all experimental conditions being the same for each measurement.
In other words, accuracy increases as data are accumulated. Typically, only one significant digit of precision
is added to x above that reported for the individual xi .
The result x can be defined in a similar fashion as Eq. (6.9), provided that the data distribution function
f (xi ) is known, namely


N
x= xi fD (xi ) . (6.23)
i=0

For instance, a given set of data can be cataloged according to the frequency of observations. The observed
frequency becomes a legitimate estimate of the probability distribution for the random variable. This ex-
perimentally determined data distribution function changes as more data are accumulated, yet converges on
the true probability distribution function as the number of sampled data points approaches infinity.

Example 6.2: Suppose a local farmer sells apples each day at the farmer’s market. He sells the following
number of apples for each day of the week, starting on Sunday and ending Saturday: 28, 14, 19, 24, 18, 21,
32. What is the sample mean for the week of sales?

Solution:
The sample mean of apples sold per day from these 7 xi ’s is found to be

1
7
28 + 14 + 19 + 24 + 18 + 21 + 32 156
x= xi = = = 22.3.
7 i=1 7 7

From the limited data set, it is concluded that the farmer sells 22.3 apples per day on average.

Example 6.3: Given two fair dice, what is the probability distribution function for expected numbers
resulting from tosses of the die compared to a an experimental distribution function composed of 100
experimental trials?

Solution:
For two dice there are 36 possible number combinations. The probability distribution function repre-
senting the summed die values and expected frequencies are shown in Table 6.1 and Fig. 6.2.

Table 6.1. Probabilities associated with throwing two dice.

Value of Thrown xi 1 2 3 4 5 6 7 8 9 10 11 12
No. of Combinations 0 1 2 3 4 5 6 5 4 3 2 1
1 2 3 4 5 6 5 4 3 2 1
f (xi ) 0
36 36 36 36 36 36 36 36 36 36 36
Sec. 6.5. Probability Data Distribution 191

Because there is no possibility of throwing a 0 or 1, the following is found.


12
0 1 2 3 4 5 6 5 4 3 2 1
f (xi ) = + + + + + + + + + + + = 1,
x=1
36 36 36 36 36 36 36 36 36 36 36 36

which is the expected result for a probability distribution function. Because the actual PDF is known, the
true mean is calculated to be
12          
0 1 2 3 4
μ(x) = xi f (xi ) = 1 +2 +3 +4 +5 +
x=1
36 36 36 36 36
             
5 6 5 4 3 2 1
6 +7 +8 +9 + 10 + 11 + 12 = 7.
36 36 36 36 36 36 36

That the expectation value is 7 is intuitively correct because the die-tossing PDF is symmetric about the
number 7.
By comparison, the data distribution function for an experiment in which 100 tosses of two dice were
observed is shown in Table 6.2 and in Fig. 6.2. Equation (6.23) is used to determine the experimental mean
Table 6.2. Observed data for 100 throws of two dice.

Value of Thrown xi 1 2 3 4 5 6 7 8 9 10 11 12
No. of Combinations 0 1 2 3 4 5 6 5 4 3 2 1
Observed Occurences 0 3 5 11 7 15 16 13 10 10 7 3
fD (xi ) .00 .03 .05 .11 .07 .15 .16 .13 .10 .10 .07 .03

of the observed data from the dice tosses, i.e.,


12
x= xi fDi = 1 (.00) + 2 (.03) + 3 (.05) + 4 (.11) + 5 (.07) + 6 (.15)
x=1
7 (.16) + 8 (.13) + 9 (.10) + 10 (.10) + 11 (.07) + 12 (.03) = 7.09

Here it is found that the sample mean x is close to the true mean μ(x). Should the experiment be conducted
again, the outcome of the experimental mean would once again be near the true mean (although not neces-
sarily the same as the previous result), and the data distribution function would be slightly different. If more
data are accumulated in the experiment, thereby increasing the number of trials N , the data distribution
function approaches that of the probability distribution function, and the experimental mean approaches
the value of the true mean.

6.5.2 Sample Median


Consider the sample median x̃ from a set of measurements x1 , x2 , ..., xN , where each xi is a non-negative
number and N represents the number of measurements taken. To find the sample median, the xi are
rearranged in ascending (or descending) order, from smallest to largest (or largest to smallest). The ordered
sequence is denoted by x(1) , x(2) , . . . , x(N ) . The sample median is defined as
$
middle value of x(i) , if N is odd
x̃ = . (6.24)
mean value of the two middle x(i) , if N is even
192 Probability and Statistics for Radiation Counting Chap. 6

Figure 6.2. The PDFs for the tossing of two dice. Left: theoretical probabilities for obtaining all possible
summed values of the dice. Right: experimental probabilities obtained after 100 throws.

Example 6.4: Revisit Example 6.2, in which a farmer sold the following number of apples in consecutive
days of a single week: x1 , x2 , . . . , xN = 28, 14, 19, 24, 18, 21, 32. Find the experimental median.

Solution:
Reordering the data from lowest to highest values produces the set
x(1) , x(2) , . . . , x(N) = 14, 18, 19, 21, 24, 28, 32.
Here N = 7 is odd and the sample median (or middle value) is represented by the 4th entry in the ordered
list, i.e., x̃ = x(4) = 21 . Notice the sample median is not equal to the sample mean found in Example 6.2.

Example 6.5: Suppose a well pumping company accumulates data regarding the lifetimes of 1/2 horse-
power pumps. Over a period of 12 years, the following failure times, in months, for 20 different pumps were
observed,
31, 29, 60, 49, 30, 95, 37, 85, 39, 47, 135, 50, 52, 21, 54, 45, 58, 12, 64, 40
What are the sample mean and median values for these data?

Solution:
The sample mean is
1 
20
1
x= xi = (31 + 60 + 29 + 49 + 30 + 95 + 37 + 85 + 39 + 47 +
20 i=1 20
1033
135 + 50 + 52 + 21 + 54 + 45 + 58 + 12 + 64 + 40) = = 51.7.
20
Hence, the average lifetime of the 1/2 horsepower pump is found to be 51.7 months. To find the sample
median, the order is arranged from smallest to largest values,
12, 21, 29, 30, 31, 37, 39, 40, 45, 47, 49, 50, 52, 54, 58, 60, 64, 85, 95, 135
Because N = 20 is even, the sample median is the average of the 10th and 11th values in the ordered list,
x(10) + x(11) 47 + 49
x̃ = = = 48.0.
2 2
It should be noticed that the sample median is close to, but not equal to, the sample mean in this case.
Sec. 6.5. Probability Data Distribution 193

6.5.3 Trimmed Sample Mean


It is common to encounter experimental data in which some measurements yield values that are quite far
from either the sample mean or sample median. Such points are commonly referred to as “outliers,” which an
analyst may regard as non-representative for the data set. Hence, it is important to notice a major distinction
between the sample mean and the sample median. The sample mean takes into account all observed values,
whereas the sample median eliminates those values that are not in the middle of the ordered distribution.
The sample mean is affected by outlying values, whereas the sample median is not affected by outlying values
at all, thereby representing two opposite extremes for interpreting the data distribution.
The sample mean uses all data values, even those from the extreme ends of the distribution, whereas
the sample median is insensitive to the extreme values at the two ends of the distribution. One method
to eliminate the outliers’ influence on the sample mean is to use a trimmed mean. As an example, a 5%
trimmed mean is computed by eliminating the smallest 5% and the largest 5% of the sample values, and
then calculating the sample mean from the remaining data.
There are instances when a standard percentage trimmed mean is prescribed, but the number of mea-
surements does not allow this to be exactly done. For instance, one might have 23 data points, in which case
a 10% trimmed mean would need to have 2.3 data points eliminated from the smallest and largest extremes
of the ordered distribution. Clearly, this is not possible. Instead, interpolation between the nearest possible
points is generally used. For instance, the 10% trimmed mean should be calculated by determining the
trimmed mean with only 2 data points removed from upper and lower portions of the distribution, and then
repeated with 3 data points removed from upper and lower portions of the distribution. The 10% trimmed
mean is determined by appropriate interpolation between the two trimmed means.

Example 6.6: The ordered data in Example 6.5 of the lifetime of pumps, in months, are

12, 21, 29, 30, 31, 37, 39, 40, 45, 47, 49, 50, 52, 54, 58, 60, 64, 85, 95, 135
It appears that some pumps had very short lifetimes (possibly due to manufacturing defects or ove use) and
some had very long lifetimes (possible due to low usage). To avoid these outliers, one should calculate a
trimmed mean, for example, a 10% trimmed mean.

Solution:
With this data censoring, the trimmed data are

29, 30, 31, 37, 39, 40, 45, 47, 49, 50, 52, 54, 58, 60, 64, 85

With only 16 data measurements remaining, the 10% trimmed mean is

1 
16
1
xtr(10) = xi = (29 + 30 + 31 + 37 + 39 + 40 + 45 + 47
16 i=1 16
770
+49 + 50 + 52 + 54 + 58 + 60 + 64 + 85) = = 48.1 months.
16
Notice that the trimmed mean is now much closer to the uncensored sample median of 48.0 months. This
result might indicate to the pump manufacturer that those pumps with lifetimes less than two years were
actually defective, and did not represent the true quality of the product.
194 Probability and Statistics for Radiation Counting Chap. 6

6.5.4 Sample Variance


Often an experimenter encounters a situation in which data about random variables have been accumulated,
yet the true probability distribution function f (x) is unknown. There are several options that might be
used to determine an informative measure of the reasonableness of a sample set. The population variance
and sample variance are dispersion indices that deal with the variability of actual data. If the true mean
μ(x) of a distribution is known, then the population variance is denoted σ 2 (x), and the population standard
deviation is σ(x), where,
1 
N
σ 2 (x) = (xi − μ(x))2 . (6.25)
N i=1

However, the actual value of μ(x) is rarely known. Instead, the experimentally observed average, x, is usually
used as an estimate of μ(x). Typically, the sample variance, denoted s2 , is used to estimate the variance in
the data distribution, where

1 
N
s2 = (xi − x)2 . (6.26)
N − 1 i=1

The sample standard deviation, denoted by s, is the positive square root of the sample variance. That
N − 1 is used in the denominator instead of N , used in the definition of the population variance, is because
all of the N xi are used to calculate x, so that only N − 1 of the xi are independent of x. In common
parlance, “one degree of freedom” is lost by using x to approximate μ(x) [Box et al. 1978]. Another way of
understanding this issue is to recall the result of Eq. (6.22). If N − 1 of the xi ’s are known, the final xi is
already determined because the summation of (xi − x) must equal zero. Hence, there are only N − 1 degrees
of freedom that can be used to determine the sample variance.

Example 6.7: A series of 30 radiation measurements are performed on a check source, each measurement
6 seconds long, to calibrate a detection system. Given the following counts as recorded for each measure-
ment, determine the sample mean, the sample variance, the sample standard deviation and plot the data
distribution function.

Solution:
Measurement data:

29, 30, 26, 33, 32, 31, 19, 35, 29, 31, 38, 25, 23, 33, 24,
28, 37, 26, 29, 41, 30, 27, 23, 34, 40, 27, 21, 30, 29, 31.

From Eq. (6.22), the experimental mean is found to be

1 
N
891
x= xi = = 29.7.
N i=1 30

The sample variance is found from Eq. (6.26)

1  1 
N 30
816.3
s2 = (xi − x)2 = (xi − 29.7)2 = = 28.15.
N − 1 i=1 30 − 1 i=1 29

The sample standard deviation is √


s= 28.15 = 5.31.
Sec. 6.5. Probability Data Distribution 195

 
        


   







 


   






     


Figure 6.3. The distribution of counts in each of the 30 measure-


ments and the difference, positive and negative, from the mean value
(x = 29.7). Also shown is a comparison with the sample standard
deviation (s = 5.31).

The sum of the differences, shown in Fig. 6.3, is zero. However, the sample variance and sample standard
deviation are non-zero. The sample standard deviation is shown in Fig. 6.3 as compared to the difference
xi − x for the 30 measurements.
The data distribution function, fD (xi ), is determined with Eq. (6.17), where each frequency of observed
counts is divided by 30. For instance, four measurements resulted in the observation of xi = 29 counts,
yielding
4
fD (xi = 29) = = 0.133.
30
The resulting histogram for the 30 measurements is plotted in Fig. 6.4. Finally, it should be noted that as
more data are accumulated, the data distribution function begins to take on the appearance of the theoretical
PDF, in this case, a Gaussian distribution.
196 Probability and Statistics for Radiation Counting Chap. 6






  


  !   "#$  


 
 












       

  %&'
Figure 6.4. The distribution of counts in each of the 30 measurements projected as a data
distribution function. The data distribution function describes the experimentally determined
probability of observing a randomly chosen number of counts per measurement.

6.6 Binomial Distribution


There are experiments in which only two outcomes are possible, hence Table 6.3. Possible outcomes of a bino-
the name binomial, which translates as meaning “two terms”. Ex- mial experiment with N = 3.
amples of binomial statistical experiments include tossing a coin for Number of
“heads” or “tails”, picking marbles of two different colors from a Outcome Probability
successes
box, uncovering shells with or without a prize underneath, and se- SSS 3 p3
lecting whether or not today is your birthday. If such an experiment, SSF 2 p2 (1 − p)
regardless of type, is conducted over N number of trials, then the SF S 2 p2 (1 − p)
possibilities of observing either one or the other result can be listed. F SS 2 p2 (1 − p)
Typically one of the possible outcomes is listed as a “success” (S) SF F 1 p(1 − p)2
FFS 1 p(1 − p)2
and the other a “failure” (F ). For instance, consider a coin toss ex- F SF 1 p(1 − p)2
periment in which exactly three trials are conducted. In such a case, FFF 0 (1 − p)3
if the outcome is a “heads” it is listed as a success, and an outcome
of “tails” is listed as a failure. For any independent set of 3 trials, there are only 8 possible outcomes, as
listed in Table 6.3.
The probability of observing a success is denoted p. Because there are only two possible outcomes from
any single trial, the probability of observing a failure must be (1 − p). Also listed in Table 6.3 are the
probabilities of achieving any of the possible combinations. For instance, the probability of achieving a
success 3 times in a row is ppp = p3 . The probability of observing an outcome for x number of times
from N trials can be determined by dividing the number of times the desired outcome can appear by the
total number of possible outcomes. Because only one outcome results in three successes, the probability of
throwing three heads in a row out of three trials is 1/23 = 0.125. Unfortunately, for a large number of trials N ,
Sec. 6.6. Binomial Distribution 197

listing all possible outcomes becomes an explosively difficult method to


use. For example, there are 1024 possible outcome combinations for 10
independent trials.
Fortunately, a Swiss mathematician Jacques Bernoulli (a.k.a. James
or Jacob) worked out a general solution to binomial experiments,3 often
referred to as Bernoulli trials, hence eliminating the need to list all pos-
sible experimental outcomes. Let p denote the probability of observing a
success for a particular event. Then the probability that the event is not
observed in any trial is q = 1 − p. In any trial one must either observe the
event or not observe the event. Thus, p + q = 1 = (p + q)N . A binomial
expansion then gives

N (N − 1) N −2 2
(p + q)N = pN + N p(N −1) q + p q
2!
Figure 6.5. Jacques Bernoulli
N (N − 1)(N − 2) N −3 3
+ p q + ... + q N = 1. (6.27) (1654–1705).
3!
Substitution of (1 − p) for q yields,

N (N − 1) N −2
(p + q)N = pN + N p(N −1) (1 − p) + p (1 − p)2
2!
N (N − 1)(N − 2) N −3
+ p (1 − p)3 + ... + (1 − p)N = 1, (6.28)
3!
which can be rewritten as,

(p + q)N = f (N ) + f (N − 1) + f (N − 2) + ... + f (0) = 1. (6.29)

Here the PDF f (x) is the probability of observing the event x (an integer) number of times in N trials. Each
individual term in Eqs. (6.28) and (6.29) can be denoted as

N!
B(x|p, N ) ≡ fB (x) = px (1 − p)N −x , x = 0, 1, 2, . . . , N. (6.30)
(N − x)!x!

In this discrete PDF (see Sec. 6.2.2), known as the binomial distribution, the random variable x assumes
non-negative integer values, i.e., x1 = 0, x2 = 1, . . ..
The binomial distribution is the governing distribution whenever the following experimental conditions
are fulfilled:

1. The experiment consists of a fixed number of N trials, where N is specified before the experiment
begins.

2. Each trial is identical in condition, and each trial can result in one of two possible outcomes. Generally,
the outcome is denoted as a success S or a failure F .

3 Late in the 17th century, Jacques Bernoulli (see Fig. 6.5) derived the binomial PDF and, of even greater importance, the law
of large numbers. These results were eventually published posthumously in 1713 by his nephew, Nicolaus Bernoulli, in Ars
Conjectandi (“The Art of Conjecture”).
198 Probability and Statistics for Radiation Counting Chap. 6

3. The trials are independent, and the outcome of each trial does not affect the outcomes of other trials.

4. The probability of a success p is the same from trial to trial.

For instance, if a test involves the probability of removing specific balls from a box (for instance, black
or white in a mixture of both), for each ball removed from the box the actual probability for the next test
has changed because a ball has been removed. For large sample sets, the resulting change in p may be small
enough to be of no consequence; however, the experimenter must review the possibility of whether or not
replacement does matter. Generally, an experiment can be approximated as being binomial provided that
the sample size, N , is less than 5% of the population size. For instance, with a box of 10,000 marbles,
extracting 500 or less marbles during the experiment can be approximated as a binomial experiment.4
For any given binomial experiment, the average number of successes observed is


N 
N
xN !
μ(x) = xB(x|p, N )) = px (1 − p)N −x . (6.31)
x=0 x=0
(N − x)!x!

Let y = x − 1 and M = N − 1; then x = y + 1 and N = M + 1, and it is easy to show N − x = M − y. Thus

M
(y + 1)(M + 1)! y+1 M
(M + 1)(M )! y
μ(x) = p (1 − p)M−y = p p (1 − p)M−y
y=0
(M − y)!(y + 1)! y=0
y!(M − y)!

M
(M )! M
= (M + 1)p py (1 − p)M−y = N p f (y|p, M )
y=0
y!(M − y)! y=0

Because the summation of a discrete PDF over all possible outcomes is unity, the above simplifies to

μ(x) = N p. (6.32)

In a similar manner, the variance of the binomial distribution is found to be

σ 2 (x) = pN (1 − p). (6.33)

Example 6.8: A simple experiment, with which most readers are familiar, is that of tossing a fair coin.
Intuitively it is known that the probability of observing a “head” or a “tail” is 50%. Suppose the observation
of a heads is determined to be a success. What is the probability that out of 10 tosses exactly 7 successes
are observed? What is the average number of successes expected from 10 coin tosses?

Solution:
For the parameters p = 0.500, x = 7, and N = 10, the probability of throwing exactly 7 heads out of 10
trials is
N! 10! 10!
B(x|0.5, 10) = px (1 − p)N−x = (0.5)7 (1 − 0.5)10−7 = (0.5)7 (0.5)3 = 0.117.
(N − x)!x! (10 − 7)!7! 3!7!

4 Notethat, while the binomial distribution is a good approximation for large sample populations, its use for small populations
without replacement can result in unacceptable error. For such small populations, the hypergeometric distribution must be
used [Devore 1991]. Because this distribution is rarely used for radiation counting, the hypergeometric distribution is not
covered here.
Sec. 6.6. Binomial Distribution 199

There is, thus, an 11.7% probability that exactly 7 out of 10 tosses result in the observation of heads.
The expected number of heads observed from 10 coin tosses is μ = pN = (10)(0.5) √ = 5. The variance is
σ 2 = pN (1 − p) = (0.5)(10)(0.5) = 2.50. Finally, the standard deviation σ = 2.50 = 1.58. Thus, for 10
coin tosses, the expected number of heads that are observed is 5.00 ± 1.58.
The expected number of successes from a binomial distribution for various values of p are shown in Table
6.4 for the condition in which N = 10. The binomial distribution becomes symmetric for p = 0.5, such
as with the coin toss example. The summed probabilities equal unity in each case, meaning that out of
10 trials, at least one of the observations in the column marked x are observed. The condition in which
p = .5 with N = 10, as with the coin toss example, is plotted in Fig. 6.6. For the case of N = 10 trials the
probabilities of different outcomes for fixed values of p are listed in Table 6.4.


 
 












            
     

Figure 6.6. The binomial distribution for the coin toss example, in
which N = 10, showing the probabilities of throwing exact numbers of
heads (successes).

6.6.1 Radioactive Decay and the Binomial Distribution


Radionuclides are governed by binomial statistics because a radionuclide either decays in a time interval t
or it does not. Consider a radioactive sample initially containing No identical radionuclides with a decay
constant λ. The probability a radionuclide does not decay in time t is (1 − p) = e−λt , so the probability it
does decay is p = (1 − e−λt ). From Eq. (6.30) the probability fB (x) that x atoms decay in time T is
No !
fB (x) = (1 − e−λT )x (e−λT )No −x x = 0, 1, 2, . . . , No . (6.34)
(No − x)!x!
From Eq. (6.32) the average number decaying in time T is
μ(x) = No (1 − e−λT ) (6.35)
and the variance is
σ 2 (x) = No (1 − e−λT )e−λT = μ(x)e−λT . (6.36)
200 Probability and Statistics for Radiation Counting Chap. 6

Table 6.4. Probabilities for the number of successes for a binomial distribution
with N = 10 and p = 0.1, 0.3, 0.5, 0.7 and 0.9.

fB (x)
x p = 0.1 p = 0.3 p = 0.5 p = 0.7 p = 0.9
0 0.348678 0.028248 0.000977 5.90 × 10−6 10−10
1 0.387420 0.121061 0.009766 0.000138 9 × 10−9
2 0.193710 0.233474 0.043945 0.001447 3.65 × 10−7
3 0.057396 0.266828 0.117188 0.009002 8.75 × 10−6
4 0.011160 0.200121 0.205078 0.0036757 0.000138
5 0.001488 0.102919 0.246094 0.102919 0.001488
6 0.000138 0.036757 0.205078 0.200121 0.011160
7 8.75 × 10−6 0.009002 0.117188 0.266828 0.057396
8 3.65 × 10−7 0.001447 0.043945 0.233474 0.193710
9 9 × 10−9 0.000138 0.009766 0.121061 0.387420
10 10−10 5.90 × 10−6 0.000977 0.028248 0.348678


If λT  1, i.e., the measurement time is very much less than the half-life of the radionuclide, σ(x) = μ(x).
Let c be the probability that a decay produces a count in a radiation detection system. Then the
probability a count is observed in time T is pc = c(1 − e−λT )  cλT if λT  1. Thus, the probability of
obtaining x counts in time T is

No !
fB (x) = (cλT )x (1 − cλT )No −x , x = 0, 1, 2, . . . , No . (6.37)
(No − x)!x!

Although, this approximation for fB (x) and the exact result of Eq. (6.34) describe the statistics of
radioactive decay, these descriptions have little utility. Because No is typically very large (105 –1015 ), the
terms involving No typically are uncalculably huge or ridiculously small. Another difficulty with using the
binomial distribution to describe radioactive decays occurs if a radioactive sample has multiple radioactive
species. In this case, the probability of obtaining x decays in time T is no longer described by a binomial
distribution. However, both of these problems are avoided by using the Poisson distribution discussed next.

6.7 Poisson Distribution


Suppose that an experimenter is observing a radiation source anticipating the emission of a radiation quan-
tum. The source contains m different radioactive species with Mi atoms and a decay constant λi for the
ith species. Assume there is negligible decay in the observation time T , i.e., λi T  1, so that the Mi do
not change appreciably. The observing time T is segmented into N smaller intervals of the same length Δt;
hence, T = N Δt. From Eq. (6.34) the probability that no atoms of species i decays in Δt is

Mi !
fB (0) = (1 − e−λi Δt )0 (e−λi Δt )(Mi −0) = e−λi Mi Δt . (6.38)
(Mi − 0)!0!
m
The probability none of the radionuclides decay in Δt is, thus, i=1 exp(−λi Mi Δt) and the probability one
(or more) radionuclides decay is

)
m
pdecay = 1 − e−λi Mi Δt = 1 − e−(λ1 M1 +...+λm Mm )Δt . (6.39)
i=1
Sec. 6.7. Poisson Distribution 201

As N → ∞, Δt → 0 and
* +

m
pdecay  λi Mi Δt, (6.40)
i=1

which also vanishes as N → ∞ with the probability of two or more decays vanishing faster than the
probability of a single decay in Δt. Now define ci as the probability of recording a count per decay of
radionuclide species i,5 so the probability of recording a count in a small Δt is
*m +

p= ci λi Mi Δt, (6.41)
i=1

Again as N → ∞, both Δt → 0 and p → 0; but the product N p remains finite, i.e., Eq. (6.41) with
Δt = T /N yields
*m + *m +
 T 
Np = N ci λi Mi = ci λi Mi T ≡ μ. (6.42)
i=1
N i=1

Thus, in the limit of large N , with p = μ/N the binomial distribution of Eq. (6.30) becomes

N! μ x μ N −x
fB (x) = lim 1− , x = 0, 1, 2, ..., N (6.43)
N →∞ (N − x)!x! N N

When N is large, the evaluation of the binomial distribution of Eq. (6.43) becomes computationally
difficult because the various factorials in the binomial coefficient become enormous. But Eq. (6.43) can be
considerably simplified as follows:

N (N − 1) · · · (N − x + 1) μx μ N μ −x
lim fB (x) = lim 1− 1−
N →∞ N →∞ N (N ) ··· (N ) x! N N
   
1 x−1
1− ··· 1 −
N N μx μ N
= lim μ x 1− . (6.44)
N →∞ x! N
1−
N
As N → ∞, the terms (1 − i/N ) and (1 − μ/N ) approach unity. Also from the properties of the base of the
natural logarithms e, it is known that

μ N
lim 1− = e−μ . (6.45)
N →∞ N

Hence Eq. (6.44), in the limit as N → ∞, yields

μx −μ
P(x|μ) ≡ fP (x) = e , x = 0, 1, 2, . . . . (6.46)
x!

5 Here it assumed that an ideal counting system is being used so that ci is a constant and unaffected by realities such as dead
time.
202 Probability and Statistics for Radiation Counting Chap. 6

This PDF with a single parameter μ, is referred to as the Poisson (pronounced /pwä-´sōn/) probability
distribution function.6 Here it is learned that the Poisson distribution can be used provided that the
probability of observing any single event is small (by comparison to N ), or p  1. Unlike the binomial PDF,
the Poisson PDF describes the radioactive decay of both a single radioactive species or a sample containing
multiple different radionuclides.
Certain properties of the Poisson distribution should be noted.
Because it is a probability distribution function, it must be nor-
malized, i.e.,
∞
(pN )x −pN
e = 1. (6.47)
x=0
x!
For a large number of trials, the average or expected number of
successes would be N p = μ. This result can be derived more
formally as follows:
∞ ∞ ∞
μx μx μy −μ
x = x e−μ = e−μ = μ e = μ. (6.48)
x=0
x! x=1
(x − 1)! y=0
y!

In a similar fashion, the variance of the Poisson distribution is


found to be
σ 2 (x) = μ. (6.49)
Figure 6.7. Siméon-Denis Poisson (1781–
1840). This is a very important property of Poisson statistics, namely
that the variance is equal to its mean, i.e., σ 2 = μ . Because the
Poisson distribution is the limiting distribution for the binomial distribution, this result is in agreement with
the limiting value of the binomial variance for large N , p small, and N p = μ. From Eq. (6.33) one has

σB2 = N p(1 − p) = μ(1 − p) = lim μ(1 − p) = σP


2
. (6.50)
p→0

Example 6.9: During harvest season, a farmer learns that approximately 1% of the corn in his field has
insects that could damage the ears. If he pulls exactly 200 corn ears from his field to inspect them, what is
the probability that he finds exactly 3 ears of corn with insects?

Solution:
The PDF governing the number of infected ears found in N tries is described by the binomial PDF
because either an ear has insects or it does not. A comparison between the binomial and Poisson methods
will be conducted. For the binomial PDF, with p = 0.01, x = 3, and N = 200, the expected probability that
three corn ears have insects for a sample set of 200 is
N! 200!
fB (x = 3) = px (1 − p)N−x = (0.1)3 (1 − 0.1)97 = 0.18135
(N − x)!x! 97! 3!
Also, the average number of ears that will have insects out of a sample of 200 ears is

μB = pN = (0.01)(200) = 2,

6 Siméon-DenisPoisson (see Fig. 6.7) published the distribution function, now named after him, in Recherches sur la probabilité
des jugements en matière criminelle et en matière civile (1837), an analysis of probability regarding the French criminal
justice system, where the Poisson distribution appears for the first and only time in his publications.
Sec. 6.7. Poisson Distribution 203


with a standard deviation of σB = pN (1 − p) = (0.01)(200)(1 − 0.01) = ±1.407.
The approximation of the binomial PDF by a Poisson PDF yields the expected probability that exactly
three ears of corns are infested as
(pN )x −pN [(0.01)(200)]3 −(0.01)(200)
fP (x = 3) = e = e = 0.18045.
x! 3!
Also, the average number of ears and the standard deviation that have insects out of a sample of 200 ears is

μP = pN = (0.01)(200) = 2 and σP = pN = (0.01)(200) = ±1.414.
Notice how well the Poisson result agrees with the true result of the binomial PDF. Fig. 6.8 shows the
resulting Poisson distribution for x = 0, . . . , 8.

Figure 6.8. The Poisson distribution for Example 6.9, showing the
expected probabilities of finding insects in specific numbers of corn
ears from a sample set of 200.

Example 6.10: A radioactive sample has a half-life of 10 years. The sample mass has N = 109 identical
radioactive atoms at time t = 0. What is the probability that exactly 120 atoms decay within a one-minute
observation period of the sample beginning at t = 0?

Solution:
Here λ = ln(2)/10 yrs = 1.3188 × 10−7 min−1 , x = 120 and N = 109 . The expected number of decays
in one minute is
p = λΔt = (1.3188 × 10−7 min−1 )(1 min) = 1.3188 × 10−7 .
The average number of decays observed within a one-minute observation period is
μP = pN = (1.3188 × 10−7 )(109 ) = 131.88 decays.
Here Poisson statistics must be used because in this case binomial statistics produce fatal overflow problems
when attempting to evaluate fB (x = 120).
(pN )x −pN 131.88120 −131.88
fP (x = 120) = e = e = 0.02096,
x! 120!
204 Probability and Statistics for Radiation Counting Chap. 6

so there is about a 2% probability that exactly 120 decays are observed in a one-minute period. Notice that
the probability distribution shown in Fig. 6.9 is nearly symmetric about the mean value. Indeed, as the
probability of observing an event decreases to small values, and the average value for observing the event
increases (a large sample set), the Poisson PDF converges on a symmetric distribution about the mean.

Figure 6.9. The Poisson distribution for Example 6.10, showing


the probabilities of observing an exact number of disintegrations
per minute from a radioactive sample initially composed of 109
radioactive atoms.

6.8 Gaussian or Normal Distribution


For large sample sets and high averages, both the binomial and Poisson distributions are cumbersome to
implement numerically. A more manageable probability distribution function is the Gaussian PDF, also
called the normal PDF. With this PDF the probability of observing an event within some dx is7
1 (x − μ)2
N (x|μ, σ) dx = √ exp − dx. (6.51)
2πσ 2σ 2
Here N (x|μ, σ) ≡ fN (x) is the PDF that has the following properties: (1) It is properly normalized, i.e.,
 ∞  ∞
1 (x − μ)2
fN (x) dx = √ exp − dx = 1. (6.52)
−∞ −∞ 2πσ 2σ 2

(2) The average value of x is


 ∞  ∞
x (x − μ)2
xfN (x) dx = √ exp − dx = μ. (6.53)
−∞ −∞ 2πσ 2σ 2

7 Independently,Adrain in 1808 and Gauss (see Fig. 6.10) a year later developed the formula for the normal distribution and
showed that experimental errors were fit well by this distribution. However, almost thirty years earlier this distribution had
been discovered by by Laplace in 1778 as he derived the extremely important central limit theorem.
Sec. 6.8. Gaussian or Normal Distribution 205

(3) The variance of the Gaussian distribution is


 ∞  ∞
(x − μ)2 (x − μ)2
(x − μ) fN (x) dx =
2
√ exp − 2
dx = σ 2 (x) = var(x). (6.54)
−∞ −∞ 2πσ 2σ
The normal distribution is ubiquitous in nature. The famous
“bell-shape” curve keeps popping up everywhere in every disci-
pline. That the normal distribution is so prevalent is explained
by the very general and powerful central limit theorem (CLT). In
words, this theorem states that if N samples zi are drawn from
any PDF with mean μ(z) and variance σ 2 (z), then the arithmetic
average z is asymptotically distributed, for large N , as √ a normal
distribution with mean μ and standard deviation σ(z)/ N . The
astonishing feature about the CLT is that nothing is said about
the distribution function used to generate the N samples of z, from
which the random variable z is formed. No matter what the dis-
tribution is, provided it has a finite variance, the sample mean z
has an approximately normal distribution for large samples. The
restriction to distributions with finite variance is of little practical
consequence because most useful PDFs have a well-defined mean
and variance.8
In radiation counting, the measured counts are governed by the
binomial distribution and well approximated by the Poisson. Be-
cause of the CLT, it is not surprising that samples from a Poisson
Figure 6.10. Carl Friedrich Gauss (1777– PDF assume a Gaussian distribution √ for sufficiently large N . A
1855).
normal distribution in which σ = μ = pN is, in fact, a very good
approximation to the Poison PDF with mean μ, especially for large μ. Shown in Fig. 6.11 is a comparison of
the Poisson distribution and the normal distribution for a mean value of 25. Thus, it is seen that the normal
distribution is a good approximation for μ as small as 25. Although the Poisson distribution is a discrete
PDF and the Gaussian distribution is a continuous PDF, the similarity between the two is unmistakable.
The basic characteristics of the continuous√ Gaussian distribution are shown in Fig. 6.12, where it has
been renormalized by multiplying fN (x) by ( 2π)σ. Data from such a distribution are routinely reported
as x ± σ where x is the average number of measured counts during a specified time period and σ is the
standard deviation of x. When an error is reported as one standard deviation (or “one sigma”) it is called
the standard error.
Another important feature of the continuous Gaussian distribution is the full width at half maximum
(FWHM), which is the width of the distribution along the abscissa where it has half the maximum value of
the distribution along the ordinate. For instance, the renormalized distribution of Fig. 6.12 has a maximum
value of 1, hence the FWHM is the change in x between the points at which the distribution equals 0.5.
The relationship between σ and the FWHM is found by evaluating fN (x ) = 0.5fN (μ), where as seen in
Fig. 6.12, |μ − x | = 0.5 FWHM. To find the FWHM write fN (x ) = 0.5fN (μ) explicitly as
1 (0.5 FWHM)2 1 1
√ exp − = √ .
2πσ 2σ 2 2 2πσ

8 One exception is the Cauchy or Lorentzian PDF, which has no mean or variance,
1 β
fC (x) = , −∞ < α < ∞, β > 0, −∞ < x < ∞.
π (x − a)2 + β 2
206 Probability and Statistics for Radiation Counting Chap. 6

Figure 6.11. A comparison of the Poisson PDF fP (xi ) and the Gaussian
PDF fN (x) for a mean value of 25. The Poisson PDF is slightly asym-
metric, whereas the Gaussian PDF is symmetric about the mean. Yet,
the Gaussian distribution is a good approximation for the Poisson PDF,
hence is commonly used as a substitute for the Poisson PDF in radiation
counting.





    



 

 




  
 


 

 

Figure 6.12. The√Gaussian, or normal, distribution function that has


been multiplied by 2πσ.

Take the log of both sides and solve for FWHM to obtain


FWHM = 2 2 ln(2)σ  2.355σ. (6.55)
Sec. 6.8. Gaussian or Normal Distribution 207

6.8.1 Standard Normal Distribution


The normal distribution of Eq. (6.51) can be changed into a more symmetric one. Let z = (x − μ)/σ so that
Eq. (6.51) becomes
1 z2
fN (z) = √ exp − ≡ fN (z|0, 1). (6.56)
2π 2
The mean of this standard normal is
 ∞  ∞
z z2
μ= zfN (z)dz = √ exp − dz = 0, (6.57)
−∞ −∞ 2π 2

and the variance is  


∞ ∞
z2 z2
2
σ (z) = 2
z fN (z)dz = √ exp − dz = 1. (6.58)
−∞ −∞ 2π 2
Here it is found that the average is 0, meaning that the distribution is centered at z = 0, and the variance
and standard deviations are both equal to unity. This particular form of the Gaussian distribution is referred
to as the standard normal probability distribution and sometimes is denoted by fN (z) ≡ N (z|0, 1).
A normal distribution N (x|μ, σ) with any μ or σ is transformed to the standard normal N (z|0, 1) by
letting z = (x − μ)/σ. By converting a normal distribution to the standard normal PDF the probability
distribution becomes “standardized,” the results of which can be found in a number of different mathematical
tables for various values of z. Hence, by converting the Gaussian distribution to the standard normal
distribution, the probabilities can be easily determined for any values of μ and σ. The standard normal PDF
is shown in Fig. 6.13.

Figure 6.13. The standard normal distribution fN (z|0, 1) is centered at z = 0 with


both σ2 and σ equal to 1. The x-axis labels are the number of standard deviations from
the mean (z = 0).
208 Probability and Statistics for Radiation Counting Chap. 6

Example 6.11: A factory produces ball bearings with an average radius of μ = 6 mm and with a standard
deviation of σ = 0.04 mm. The diameters of the ball bearings must not be any less than 5.9 mm nor larger
than 6.1 mm in order to fit into the sleeves for which they were designed. Out of a daily manufacture run
of 20,000 ball bearings, how many ball bearings must be rejected?

Solution:
Good ball bearings fall between the diameters of 6 mm ±0.1 mm, hence, the rejected ball bearings
have radii in the intervals (0, 5.9) mm and (6.1, ∞). Here it is assumed that a normal PDF describes the
distribution of radii. Although negative radii are unphysical, the area under the Gaussian tail of (−∞, 0) is
negligibly small and totally ignorable here. Thus

Prob{x < 5.9mm} + Prob{x > 6.1mm} =


 5.9  ∞
1 (x − 6)2 1 (x − 6)2
√ exp − dx + √ exp − dx
−∞ 2π 2(0.04)2 6.1 2π 2(0.04)2

To evaluate these two integrals, convert the normal PDF to the standard normal PDF by substituting
x−μ x−6
z= =
σ 0.04
so that the acceptance limits become
5.9 − 6 6.1 − 6
zlow = = −2.5 and zhigh = = 2.5.
0.04 0.04
Because the Gaussian distribution is symmetric about the mean, it is necessary to calculate the probability
of finding ball bearings within only one of these intervals, and afterwards simply doubling the answer. Thus,
to find probability in the interval (2.5, ∞) integrate the standard normal PDF between −∞ and 2.5 and
subtract the results from 1 as shown in Fig. 6.14.
 ∞
1 z2
Prob{x < 5.9mm} + Prob{x > 6.1mm} = 2 √ exp − dz
2.5 2π 2
 2.5
1 z2
=2 1− √ exp − dz .
−∞ 2π 2

The value of the last integral is easily found from a table of the standard normal PDF, where it is found
 2.5
1 z2
√ exp − dz = 0.99379.
−∞ 2π 2

Hence the probability a ball bearing is rejected is

Prob{x < 5.9mm} + Prob{x > 6.1mm} = 2 [1 − 0.99379] = 0.01242.

It is, thus, expected that (20, 000)(0.01241) = 248.4 ball bearings must be rejected each day.
Sec. 6.8. Gaussian or Normal Distribution 209






 2.5 1  z2 


1 exp  dz
 2 2

  


        

Figure 6.14. The standard normal PDF of Example 6.11, showing the
probability region between 2.5 and ∞.

6.8.2 Cumulative Normal Distribution and the Error Function


The cumulative normal distribution has a special importance for a variety of mathematical applications. It
is defined as  y
1 (x − μ)2
FN (y) = √ exp − dx. (6.59)
−∞ 2πσ 2σ 2
Notice that the FN (y) is the probability of observing an event between −∞ and some specified value y.
This cumulative normal distribution can be converted to the cumulative standard normal distribution by
using again the substitution z = (x − μ)/σ to give
 u
1 z2
FN (u) = √ exp − dz. (6.60)
−∞ 2π 2

The above integration of the standard normal distribution is shown in Fig. 6.15.
A function closely related to the CDF of the standard normal distribution is the error function, defined
as  u
2  
erf(u) = √ exp −z 2 dz. (6.61)
0 π
Because the standard normal PDF is symmetric about the origin, the relationship between the error function
and the cumulative standard normal distribution is, for u > 0,
 u  
1 1 z2 1 u
FN (u) = + √ exp − dz = 1 + erf √ . (6.62)
2 0 2π 2 2 2

For any positive value of the product uσ ≡ u σ, erf(uσ / 2σ) is the probability that the error of a single
measurement lies between −uσ and +uσ . Because σ = 1 for the standard normal distribution, the probability
210 Probability and Statistics for Radiation Counting Chap. 6


interval between ±σ is erf(1/ 2) = 0.683. This is the same probability of observing x from N (x|μ, σ) in the
interval [μ − σ, μ + σ]. A comparison of the functions FN (u) and erf(u) is shown in Fig. 6.16.


 

1u  z2
  2
exp 
 2
dz
   






        


Figure 6.15. The cumulative standard normal distribution showing the prob-
ability region up to the value of u (shaded area).






 u 

erf  
 2






 FN (u )





        

Figure 6.16. A comparison of the cumulative standard
√ normal distribution
FN (u) of Eq. (6.59) and the error function erf(u/ 2) given by Eq. (6.61).
Sec. 6.8. Gaussian or Normal Distribution 211

Example 6.12: Use the error function to calculate the probability of observing x in the interval [μ −
mσ, μ + mσ] for m = 0.5, m = 1.5, and m = 2.5.

Solution:
The probability is
     
uσ u·σ u
Prob{μ − mσ ≤ x ≤ μ + mσ} = erf √ = erf √ = erf √ .
2σ 2σ 2
Here u equals 1.5, 2.5 and 2.5. From error function tables,
 
0.5
Prob{μ − 0.5σ ≤ x ≤ μ + 5σ} = erf √ = erf(0.354) = 0.383
2
 
1.5
Prob{μ − 1.5σ ≤ x ≤ μ + 1.5σ} = erf √ = erf(1.061) = 0.866
2
 
2.5
Prob{μ − 2.5σ ≤ x ≤ μ + 2.5σ} = erf √ = erf(1.768) = 0.988.
2

6.8.3 Discrete Gaussian Distribution


The previous sections about the normal PDF have described continuous functions. However, for radiation
counting, either the presence of a radiation disintegration (or count) is observed or it is not. In other words, a
fraction of an event can never be observed. The Poisson PDF is a discrete distribution that is a better model
for describing radiation counting statistics; however, it is numerically difficult to use for large numbers of
counts. Thus, one is forced to use the normal PDF. Because only discrete integers of counts can be observed,
it, therefore, becomes necessary to use the discrete Gaussian distribution to describe sample populations.
The discrete Gaussian distribution is defined, measured and analyzed only at integer values xi of counts,
although the mean μ is not necessarily an integer. This discrete distribution is normalized, i.e.,


fN (xi ) = 1, (6.63)
i=1

where, because the normal PDF approximating the Poisson has σ 2 = μ,

1 (xi − μ)2 1 (xi − μ)2


fN (xi ) = √ exp − 2
=√ exp − . (6.64)
2πσ 2σ 2πμ 2μ

It is actually the discrete form of the Gaussian distribution that is observed for radiation counting
experiments. The observations of counts must be either null or positive discrete numbers, yet the mean,
standard deviation, and variance are determined from the accumulated data and may take on any value
between 0 and ∞, because they are not necessarily integers.
Suppose an experimenter has a radioactive source used for calibration, such as 137 Cs. During a single
measurement over some time interval, the experimenter observes 42 counts. Because there is only one
measurement, the observed number of counts in the measurement also serves as the mean; hence as a first
estimate σ 2 = μ = 42. Ignore background counts for the moment, so from this single measurement, the
distribution is expected to follow a Gaussian PDF as shown in Fig. 6.17.
212 Probability and Statistics for Radiation Counting Chap. 6

The distribution of Fig. 6.17 shows the expected probabilities fN (xi ) of observing
%∞ various numbers of
counts, based on an average of 42 counts. The summed values of the probabilities i=1 fN (xi ) = 1. Should
the experimenter take a second identical measurement, according to the results in Fig. 6.17, there is a 6.16%
probability of once again observing 42 counts, meaning that there is a 93.84% probability that 42 counts will
not be observed. Should the experimenter take another measurement, it would most likely be some other
number than 42, and combining the two results would produce a new estimate of the mean μ  x.
Suppose the experimenter continues to take measurements under identical conditions, tallying the number
of times, or probability, each time a particular number of counts in a measurement is observed. The data
average, from Eq. (6.22), would change with each measurement. After numerous measurements (perhaps
a hundred or so), the experimenter should notice that the experimentally observed distribution approaches
that described by Eq. (6.64) with the observed new average μ  x, defined by Eq. (6.22), and with σ 2  s2
defined by Eq. (6.26).

  

 
  















     
 
Figure 6.17. The discrete Gaussian (normal) distribution determined for
a single observed measurement with 42 counts.

6.8.4 The Normal Distribution in Radiation Measurements


For a single measurement in which x counts are observed, the mean
√ value
Table 6.5. Standard deviation (%)
is estimated as x with an estimated standard deviation of σ = x; hence of count data measured with a ra-
diation detector operating in pulse
the reported value is x±σ. If a Gaussian distribution can approximate the mode.
data, then σ has a specific meaning, namely, there is a 68.3% probability
that the next observed measurement has a value that falls within the Observed Standard Deviation
Counts (1-σ error)
range x ± σ. Table 6.5 lists the relationship between the number of
radiation induced counts recorded and the percent standard deviation. 100 10%
400 5%
Thus to obtain a standard error of 1% or less requires recording at least 1100 3%
10,000 gross counts. 2500 2%
For a single radiation measurement, the counts observed are a good 10000 1%
first estimate of the number of counts that would be observed in a second
Sec. 6.8. Gaussian or Normal Distribution 213

independent measurement. If the counts observed are greater than approximately 25, a normal PDF can be
used to model the expected results. Hence, with x being the gross number of counts observed in the single
measurement, the mean and standard deviation are, respectively,

x=x and σ(x) = x. (6.65)

This result would then be reported as “counts = x ± x.” Often it is preferred that the standard deviation σ
be reported in terms of a relative to mean (fraction of the mean) or as a percent of the average, respectively
given by, √ √
x 1 x 100
σrel = = √ and σ% = 100 = √ . (6.66)
x x x x
Typically, the measurement is reported as “counts = x ± σrel ” or “counts = x ± σ% .”

Example 6.13:
A radiation measurement is conducted in which the gross counts observed are 258. How should the
counts be reported in terms of absolute, fractional and percent standard errors?

Solution:
With the above results one has
√ √
counts = x ± x = 258 ± 258 = 258 ± 16.1 absolute.
1 1
counts = x ± √ = 258 ± √ = 258 ± 0.0622 relative.
x 258
1 1
counts = x ± 100 √ = 258 ± 100 √ = 258 ± 6.22% percentage.
x 258

Uncertainties are not always reported as one standard deviation. Table 6.6. Probability intervals rela-
Sometimes a larger uncertainty is reported in order to increase the tive to the number of standard deviations
probability that the mean is included within the range between x−kσ based upon the Gaussian distribution.
and x + kσ. As shown in Table 6.6, if the error is reported as one No. of standard Probability event
standard deviation, the probability is 68.3%. However for an error deviations kσ observed in ±kσ
range of x − 1.65σ to x + 1.65σ the probability increases to 90%. 0.683σ 0.500
This new interval would be reported as the 90% confidence interval. 1.000σ 0.683
However, the convention is to report errors as one standard deviation. 1.645σ 0.900
1.960σ 0.950
For anything other than one standard deviation, one should specify 2.000σ 0.955
the number of standard deviations or the confidence interval. 2.576σ 0.990
Lastly, the shape of full-energy peaks observed from gamma-ray 3.000σ 0.997
spectra are typically Gaussian. Figure 6.18 shows a common gamma- 3.291σ 0.999
22 4.000σ 0.99994
ray spectrum from a Na source, which emits 511-keV annihilation
5.000σ 0.999999
photons from positron emissions, and 1.28-MeV gamma rays. On
comparing Fig. 6.18 to Fig. 6.12, one can observe that the photon energy peaks are Gaussian in shape.
The Gaussian shaped peaks arise from statistical fluctuations in the number of free signal carriers (charge
carriers) excited per monoenergetic photon interaction event.9 Typically the resolution of the gamma-ray

9 Thedetails regarding signal formation in gamma-ray spectrometers are addressed in the chapters on scintillation and semi-
conductor detectors.
214 Probability and Statistics for Radiation Counting Chap. 6

Figure 6.18. Differential pulse height distribution of the gamma rays emitted by the radioactive
decay of 22 Na as measured by a NaI(Tl) scintillation detector. 22 Na is a positron and gamma-
ray emitter, hence shown are the 511-keV full-energy peaks from positron annihilation and the
1.28-MeV γ ray emissions. In addition to the two full-energy peaks, several other features are also
apparent. The end points of continua for Compton scattered photons are shown, referred to as
“Compton edges”, one for the 511-keV annihilation photons and one for the 1.28-MeV γ rays. The
backscatter peak arises from 22 Na emissions scattering in the material surrounding the detector,
and then entering and interacting in the NaI detector.

peak from the detector is quoted as a function of the full peak width at half the maximum value (FWHM),
which for a Gaussian distribution is 2.355σ, where σ is in units of energy. In terms of percent, the energy
resolution is found by dividing 235.5σ by the gamma-ray energy. A detailed discussion on these matters
follows in the chapter on spectroscopy.

6.9 Error Propagation


A measurement, generally, may have several sources of error, all of which may be of such importance that they
cannot be ignored. It becomes necessary to understand how each random variable affects the measurement
error and, moreover, how such measurement error can be calculated from the values of the observed variables
[Bevington and Robinson 1992; Taylor 1997]. The usual method to estimate the error of a function of the
measured variables is to propagate the errors in each variable.
For a function described by f (x) ≡ f (x1 , x2 , x3 , ..., xN ), where the x = {x1 , x2 , ..., xN } are random
variables, the variables are usually measured quantities used to determine some average value of the random
variable f . For instance, it is common practice to perform a background measurement, with no radiation
source present, after performing a measurement on a suspected radiation source. The counts observed in the
background measurement are subtracted from the counts observed from the radiation source measurement.
Sec. 6.9. Error Propagation 215

However, both measurements have an uncertainty or standard error associated with them. What then is the
error for the difference between the counts in these two measurements?
To estimate the standard deviation of f in terms of the standard deviations σ(xi ) of the xi , it is necessary
to “propagate” these errors. The usual way to develop such an error propagation formula is to begin by
expanding f (x) in a Taylor series about the mean values of the xi , namely about the μ = {μ1 , μ2 , . . . , μN }.
Such an expansion can be written as10

∞  ∞ ∞
∂ i1 ∂ i2 ∂ iN 
f (x) 
f (x1 , x2 , . . . , xN ) = ... i1 i2 . . . iN i !, i !, . . . , i ! 
∂x1 ∂x2 ∂xN 1 2 N
i1 =0 i2 =0 iN =0 x=μ

×(x1 − μ1 )i1 (x2 − μ2 )i2 . . . (xN − μN )iN . (6.67)


Now assume that higher order terms are negligibly small so that only the first two terms are retained.
With this assumption the Taylor series reduces to

N
∂f (μ)
f (x)  f (μ) + (xi − μi ) , (6.68)
i=1
∂xi
where the notation 
∂f (μ) ∂f (x) 
≡  ,
∂xi ∂xi 
x=μ
is used. Let a0 = f (μ1 , μ2 , ..., μN ) and ai = ∂f /∂xi |x=μ . The average or expected value of f (x) is calculated
from Eq. (6.68) as
, N - 
N
E(f ) ≡ f  = a0 + (xi − μi )ai = a0  + ai xi − ai μi 
i=1 i=1

N 
N
= a0 + ai xi − ai μi  = a0 + ai (μi − μi ) = a0 .
i=1 i=1

Thus, it is seen that f  = f (μ).


Now, what of the error? The variance of F is determined as follows:
. $* + /2 0 . * N +2 0

N 
σ (f ) ≡ (f (x) − f (μ))  
2 2
a0 + (xi − μi )ai − a0 = (xi − μi )ai
i=1 i=1
. 0

N 
N 
N
= a2i (xi − μi )2 + ai aj (xi − μi )(xj − μj )
i=1 i=1 j=1
j=i


N 
N 
N
= a2i (xi − μi )  + 2
2
ai aj (xi − μi )(xj − μj )
i=1 i=1 j=1
j<i
N 
 2 
N 
N
∂f (μ) ∂f (μ) ∂f (μ)
= σi2 +2 2
σij . (6.69)
i=1
∂xi i=1 j=1
∂xi ∂xj
j<i

10 For a Taylor series to exist, it is necessary for f to be continuous and possess derivatives of all orders.
216 Probability and Statistics for Radiation Counting Chap. 6

Here σij is the covariance defined as


cov(xi , xj ) ≡ σij
2
= (xi − μi )(xj − μj ). (6.70)
Equivalently, the covariance is given by
cov(xi , xj ) = xi xj  − μi μj . (6.71)
Although determination of the covariance is important in cases where the variables are correlated, the result
is dependent upon the units of measure. Hence, the same covariance can vary widely by simply changing
the units from, for example, mm to cm. To remedy the issue, a scaling factor is used to produce a more
meaningful result, referred to as the correlation coefficient,
cov(xi , xj )
ρij ≡ , (6.72)
σi σj
where σi ≡ σ(xi ) and σj ≡ σ(xj ). Substitution of Eq. (6.71) into Eq. (6.72) yields,
xi xj  − μi μj
ρij = . (6.73)
σi σj
and Eq. (6.69) becomes
N 
 2 
N 
N
∂f (μ) ∂f (μ) ∂f (μ)
σ 2 (f ) = σi2 ) + 2 ρij σ 2 (x̂i )σ 2 (x̂j ). (6.74)
i=1
∂xi i=1 j=1
∂xi ∂xj
j=i

But how is one to use this formula since the μi are generally not known? It is usual to use the measured
values x̂i as an estimate of μi . In many situations, such as radiation measurements, it is often assumed,
usually justifiably, that the experimentally observed random variables are independent so the covariances
are zero. With these two simplifications, Eq. (6.74) reduces to the following error propagation formula:

N 
 2 
∂f (x) 
σ 2 (f ) =  σ 2 (x̂i ). (6.75)
∂xi 
i=1 xi =x̂i

If the xi are radiation counts that can be described by Gaussian distributions, then σ 2 (xi )  σ 2 (x̂i ) = x̂i .
The “error propagation formula” of Eq. (6.75) can be used provided that
1. the function can be expressed as a Taylor expansion in which the first two terms adequately approximate
the function, and
2. the variables are truly independent of each other so that the covariance between the variables is zero
(or, at least, negligibly small).
The second requirement can be usually verified by understanding the details of the physics and the
measurement systems used to obtain the measurements x̂i . However, the first requirement is generally more
difficult to verify, especially if f is highly non-linear or even if f depends very sensitively on one or more of
the x̂i .
There are a few common situations frequently encountered in radiation counting where the error propaga-
tion formula is used. These are discussed in the following subsections. For clarity, in the following examples
of error propagation a “measurement” refers to a single experiment in which a number of radiation “counts”
is observed over a preset period of time.
Sec. 6.9. Error Propagation 217

6.9.1 A Measurement is Scaled by a Constant


There are measurements in which the end result must be scaled by a constant. For instance, consider the
case
f (x) = Ax,
where A is a constant and x is the number of counts in the measurement. With the error propagation
formula, Eq. (6.75), and because σ 2 (x̂) = x̂ for a single radiation measurement, one obtains
1 
 2  2 
∂f (x i ) ∂(Ax) 
σ 2 (f ) = σ 2 (x̂i ) =  σ 2 (x̂) = A2 σ 2 (x̂). (6.76)
∂ x̂i ∂x 
i=1 x=x̂

Thus, the standard deviation of a random variable multiplied by a constant is

σ(f ) = Aσ(x̂). (6.77)

Hence, it is found that the standard error of the initial measurement is simply scaled by the constant.

Example 6.14: Suppose an experimenter wished to scale the counts obtained in a radiation measurement.
A good example is when the counts were taken for a non-standard time period, and the experimenter wishes
to scale the counts to a standardized period. For instance, if the measurement lasted 6 minutes and x̂ = 3078
counts were observed. What number of counts and standard error should the experimenter report if the
measurement times had been 60 minutes?

Solution:
The scaling factor A would be 10 in order to change the time from 6 to 60 minutes. Thus the 60-minute
measurement would produce

f (x̂) = A x̂ = (10)(3078 counts) = 30780 counts,

where x̂ is the total gross counts observed in the 6-minute measurement. From the error propagation formula

σ(f ) = Aσ(x̂) = (10) 3078 = 554.8 counts.

The expected counts and standard error for a 60-minute measurement time are then reported as

Ncounts = 30780 counts ± 554.80 counts.

Had the experimenter


√ actually counted for one hour and recorded 30780 counts, the standard error would
have been ± 30780 = ±175.4. It is, thus, important to note that the scaled standard error is larger than it
would have been had the experimenter actually performed a one-hour measurement. This outcome reinforces
the fact that the total number of observed counts determines the statistical error, and not the count rate.
Whether the experimenter performed the measurement for one minute or one hour, the average count rate
remains the same. Yet, accumulating more observed counts in a measurement reduces the overall error in
the measurement.
218 Probability and Statistics for Radiation Counting Chap. 6

6.9.2 Random Variables are Added or Subtracted


There are circumstances in which two independent variables must be added or subtracted. Consider a
function
f (x) = a1 x1 ± a2 x2 ± ... ± aN xN ,
where x1 through xN are independent random variables and the ai are arbitrary constants. With the error
propagation formula of Eq. (6.75) and measured values x̂i , the estimate of the variance of f is
N 
 2 N 
 2 
N 
N
2 ∂f (x̂i ) 2 ∂(±ai x̂i ) 2 2 2
σ (f ) = σ (x̂i ) = σ (x̂i ) = (±ai ) σ (x̂i ) = a2i σ 2 (x̂i ).
i=1
∂ x̂i i=1
∂ x̂i i=1 i=1

Therefore, the standard deviation of random variables either added or subtracted is the sum square of the
absolute variances, i.e.,


N
σ 2 (f ) = a2i σ 2 (x̂i ). (6.78)
i=1

Example 6.15: In most radiation counting environments, there is an ever present background radiation
field that can interfere with radiation measurements. To correct for this background, a measurement is
first taken with the suspected radiation source present, and then a second measurement is taken with the
suspected radiation source removed. If the measurement duration times are the same for both measurements,
then neither needs be scaled for different measurement times. The results of the second measurement, referred
to as a background measurement, is subtracted from the first measurement that recorded the summed counts
from both the suspected radiation source and the background radiation. It is necessary to report the error
for the net counts Nnet observed. Consider the case

f (x) = f (B, G) = G − B,

where G is the initial radiation measurement of gross counts and B is the background measurement. The
background measurement B is subtracted from the gross measurement G to determine the net measurement
of counts from only the radiation source. However, both G and B have error associated with their mea-
surements, and both contribute to the error in Nnet . Suppose that radiation measurements of a source and
background yield G = 2032 counts and B = 256 counts. What are the net number of counts?

Solution:
The average net counts are Nnet = G−B = 2032 cts−256 cts = 1776 cts. Because ∂f /∂G = ∂f /∂B = 1,
the error propagation formula of Eq. (6.75) yields
1
2 2
2  √ √
σ(Nnet ) = 3 σi2 = σ 2 (G) + σ 2 (B) = G + B = 2032 + 256 = 47.83 cts.
i=1

The net counts and standard error are then reported as

Nnet = 1776 cts ± 47.83 cts.


Sec. 6.9. Error Propagation 219

6.9.3 Random Variables are Multiplied or Divided


Under some situations, random variables must be either multiplied or divided. First consider the multipli-
cation case, in which
)
N
f (x) = ax1 x2 . . . xN = a xi ,
i=1

where the xi are independent random variables with measured value x̂i and a is some constant. Because
σ 2 (x) = x, the error propagation formula, Eq. (6.75), gives
N 
 2  2  2
∂f ∂ ∂
σ 2 (f ) = σi2 = (ax1 x2 ...xN ) σ12 + . . . + (ax1 x2 ...xN ) σN2

i=1
∂xi ∂x1 ∂xN
⎡ ⎤2 ⎡ ⎤2 ⎡⎛ ⎞2 ⎤
⎢ )N
⎥ 2 ⎢ )N
⎥ 2 
N
⎢⎜ ) N
⎟ 2⎥

= ⎣a ⎥ ⎢
xi ⎦ σ1 + . . . + ⎣a ⎥
xi ⎦ σN = ⎢⎜ a x ⎟ σj ⎥ .
⎣⎝ i ⎠ ⎦
i=1 i=1 j=1 i=1
i=1 i=N i=j

Now divide both sides by f 2 (x) to get the sum square of the relative variances,
 2 N  2 2

σ(f ) σ i
= . (6.79)
f (x1 , . . . , xN ) i=1
xi

Now consider the division case, in which a product of random variables is divided by another product of
random variables,
g(x) axg1 xg2 . . . xgN
f (x) = ≡ , (6.80)
h(x) xh1 xh2 . . . xhM
where xgi and xhj are independent random variables. From Eq. (6.79),

σ 2 (g)  σ 2 (xgi )  σgi σ 2 (h)  σ 2 (xhj )  σhj


N 2 N M 2 M
= 2 = 2 and = 2 = 2 . (6.81)
g 2 (x) i=1
xgi x
i=1 gi
h2 (x) j=1
xhj x
j=1 hj

Application of the error propagation formula of Eq. (6.75) to Eq. (6.80) yields,
 2  2  2  2
∂f ∂f 1 g(x)
2
σ (f ) = 2
σ (g) + 2
σ (h) = σ (g) + − 2
2
σ 2 (h). (6.82)
∂g(x) ∂h(x) h(x) h (x)

Divide both sides by f 2 (x) to obtain


 2  2
σ 2 (f ) σ(g) σ(h)
= + , (6.83)
f 2 (x) g(x) h(x)

and substitution of the terms from Eqs. (6.81) yields

σ 2 (f )  σgi  σhj
N2 2 M
= + . (6.84)
f 2 (x) x2
i=1 gi
x2
j=1 hj
220 Probability and Statistics for Radiation Counting Chap. 6

This is essentially the same result as Eq. (6.79). For multiplied or divided random variables, it is thus
concluded that the general expression for the variance, based on measured values of the random variable,
i.e., xi → x̂i , is
* +
N
σ(x̂i )
2
2 2
σ (f ) = f (x̂1 , . . . , x̂N ) . (6.85)
i=1
x̂i

Example 6.16: Suppose that the activity of a small unknown source is to be determined. One popular
method to do this is to compare it to a similar small source of known activity. For example, a calibrated
source is measured for a specified time. Afterwards, an uncalibrated source of the same type is placed in
the identical location and measured for the same amount of time. A background measurement is then taken
for the identical time period. What is the activity and standard error of the uncalibrated source given the
following data?
Calibrated source activity (Ac ): 0.9 μCi
Calibrated source measurement (Gc ): 11280 counts
Unknown source measurement (Gu ): 14560 counts
Background measurement (B): 120 counts

Solution:
The average value of the unknown activity is

Gu − B
f (x) ≡ Au = Ac
Gc − B

where Gu is the uncalibrated source measurement, Gc is the calibrated source measurement, B is the
background measurement, Ac is the activity of the known source and Au is the activity of the unknown
source.
Gu − B 14560 cts − 120 cts
Au = Ac = 0.9 μCi = 1.165 μCi.
Gc − B 11280 cts − 120 cts
The error propagation formula is used to find the standard error. For a first approximation, assume
that the background has a negligible effect on the standard error of Au . Because the variance of a single
measurement is the observed number of counts, the error propagation formula yields
 * +1/2  
2 2 1/2
σ(xu ) σ(xc ) xu xc
σ(Au )  A2u + = A2u + 2
xu xc x2u xc
  1/2   1/2
1 1 1 1
= A2u + = (1.165 μCi)2 +
xu xc 14560 cts 11280 cts

= 0.0146 μCi

The measured activity and standard error are then reported as

Au = 1.165 μCi ± 0.0146 μCi.


Sec. 6.9. Error Propagation 221

6.9.4 Random Variables in Exponents or Logarithms


The emission rate of a radiative source decreases exponentially, and it is common to encounter situations
in which the uncertainty of exponentials and logarithms of random variables must be determined. Consider
the case
f (x) = eax , (6.86)
where x is a random variable and a is a constant.11 From the error propagation formula, Eq. (6.75), one has

1  2  2
∂ ∂ ax̂ : ;2
σ 2 (f ) = f (x̂i ) σ 2 (x̂i ) = e σ 2 (x̂) = aeax̂ σ 2 (x̂). (6.87)
i=1
∂ x̂i ∂ x̂

Therefore, the standard deviation for an exponential function is

σ(f ) = a exp[ax̂]σ(x̂). (6.88)

For logarithmic functions,


f (x) = ln(ax),
where x is a random variable and a is a constant. With the error propagation formula, Eq. (6.75), one has

1  2  2
∂ ∂
σ 2 (f ) = f (x̂i ) σ 2 (x̂i ) = ln (ax̂) σ 2 (x̂) = x̂−2 σ 2 (x̂).
i=1
∂ x̂i ∂ x̂

Therefore, the standard deviation for a logarithmic function is

σ(f ) = σ(x̂)/x̂. (6.89)

Example 6.17: The total attenuation coefficient can be estimated with a simple, counting experiment.
A radiation measurement G1 is made from a source with no attenuator present, and a second measurement
G2 , of equal duration, is repeated with an attenuator of known thickness t placed between the source and
detector. Because radiation is exponentially attenuated, the two measurements are related by

G2 = G1 e−xt

where x is the attenuation coefficient. Solving for x, one obtains


 
1 G1 1
x = ln = [ln(G1 ) − ln(G2 )] .
t G2 t

Suppose the following values are observed: t = 1.5 mm, σ(t) = 0.05 mm, G1 = 1500 cts, and G2 = 1235 cts.
Estimate the attenuation coefficient.

11 Caution should be exercised here, mainly because the exponential function is highly non-linear. As a result, the first two
terms of the Taylor expansion may not adequately describe f (x). The reader is advised to refer to Section 6.9.7.
222 Probability and Statistics for Radiation Counting Chap. 6

Solution:
The linear attenuation coefficient is thus estimated as
1
x̂ = [ln(1500) − ln(1235)] = 0.1296 mm−1 .
1.5
The variance is found from the error propagation formula as
 2
2 ∂ 1
σ (x̂) = [ln(G1 ) − ln(G2 )] σ 2 (t)
∂t t
 2  2
∂ 1 ∂ 1
+ [ln(G1 ) − ln(G2 t)] σ 2 (G1 ) + [ln(G1 ) − ln(G2 )] σ 2 (G2 )
∂G1 t ∂G2 t
 2  2  2
1 1 1
= − 2 [ln(G1 ) − ln(G2 )] σ 2 (t) + σ 2 (G1 ) + − σ 2 (G2 )
t G1 t G2 t
 2  2
: ;2 1 1
= −(1.5)−2 [ln(1500) − ln(1235)] (0.05)2 + (1500) + − (1235)
(1500)(1.5) (1235)(1.5)
= 6.75 × 10−4 mm−2 .

The standard error for the measured linear attenuation coefficient is σx̂ = 6.75 × 10−4 = 2.6×10−2 mm−1 .
Hence, linear attenuation coefficient is reported to be x = 0.1296 ± 0.026 mm−1 .

6.9.5 A Series of Radiation Measurements


Quite often a series of radiation counts is conducted rather than a single measurement. For instance, the
variance about the average in a series might reveal the “goodness” of the data.12 Here it is assumed that a
consecutive series of counts x̂i is taken in which the conditions for each measurement are identical (counting
time, source position, etc.). What then is the total standard error in the sum of all the measurements? The
sum of the independent random variables xi , itself another random variable, is


N
f (x1 , . . . , xN ) ≡ xsum = x1 + x2 + ... + xN = xi
i=1

With the error propagation formula of Eq. (6.75) and the measured values x̂i , the variance of the sum is

N  2
2 ∂
σsum = xi σ 2 (x̂i ) = (1)2 σ 2 (x̂1 ) + (1)2 σ 2 (x̂2 ) + ... + (1)2 σ 2 (x̂N ) = x̂1 + x̂2 + ... + x̂N = x̂sum .
i=1
∂ x̂i

This is an important result because it shows that the variance of the sum is dependent upon only the total
number of radiation counts observed and not the number of measurements taken! Hence, the total value
of xsum determines the error, whether it is from a single measurement or a series of many measurements.
In other words, there is no appreciable difference in the error observed from a single long measurement
accumulated over some time t, or a series of N measurements in which each individual measurement is taken
for a time t/N .

12 The goodness of data refers to the correlation between the expected data fluctuations and the observed data fluctuations.
This concept is covered in Section 6.10.
Sec. 6.9. Error Propagation 223

What then is the error in the average of the N counts? Again, it is assumed that the conditions for each
measurement are identical. The average of the counts is

1  xi N
x= (x1 + x2 + ... + xN ) = .
N i=1
N

Again use the error propagation formula to determine the variance of this average,

N  2
1  2 1 
N
∂ xi x
σ 2 (x) = σ 2 (x̂i ) = 2 σ (x̂i ) = 2 x̂i = .
i=1
∂ x̂i N N i=1 N i=1 N

Thus, the standard deviation of an average of a set of measurements is

 N 1/2
x 1 
σ(x) = = x̂i . (6.90)
N N i=1

When N = 1, Eq. (6.90) reduces


√ to Eq. (6.65). For N replicate measurements, the error in the average
observed count is reduced by N . This result assumes, of course, that the measurements are independent
and that no changes occur in the radiation field or with the detector’s response during the time that the N
data points are recorded. If another series of N measurements were to be taken, a new average value for
x would be found; yet there would be a 68.3% chance that the new average would fall within the interval
ranging from x−σx and x+σx from the first series of measurements. The average number of counts observed
per measurement and standard error for N measurements is

x
x ± σ(x) = x ± . (6.91)
N

Example 6.18: An experimenter makes five identical and independent radiation measurements, each two
minutes, and records the counts 1207, 1167, 1235, 1193, and 1243. What is the average expected number of
counts per minute and the standard error?

Solution:
The average counts observed per measurement is

N
Gi 1
G= = (1207 + 1167 + 1235 + 1193 + 1243) = 1209 counts.
i=1
N 5

From Eq. (6.90),


< 
G 1209
σ(x) = = = 15.55 counts.
N 5
Division by 2 yields the average expected counts per minute and error as 604.5 ± 7.77 cpm.
224 Probability and Statistics for Radiation Counting Chap. 6

6.9.6 Measurements Over Different Time Intervals


Statistical error in radiation counting is determined Table 6.7. Comparison of errors for measurements with dif-
by the total number of counts observed during a ferent measurement times but with the same count rate.
measurement or series of measurements. However, Observed Count Standard Standard Count
there may be cases in which the measurements are counts G time t error σ error % rate g
not all taken over the same period of time. What 100 10 s ± 10 10% 10 cps
then is the error? It is incorrect to simply use the er- 1000 100 s ± 31.6 3.16% 10 cps
ror of a count rate. Instead, the experimenter must 10000 1000 s ± 100 1% 10 cps
first determine the error of the total counts observed 100000 10000 s ± 316 0.316% 10 cps
and convert that result into a count rate. To illus-
trate this, consider an experimenter who takes four different measurements over four different measurement
times producing the results shown in Table 6.7. All four measurements represent the same count rate, but
the error in each is tremendously different.
The count rate for the ith measurement is given by gi = Gi /ti . The average count rate for N independent
measurements of the same radiation source is


N &
N
f (x) ≡ g(G1 , . . . , Gn , t1 , . . . , tn ) = Gi ti . (6.92)
i=1 i=1

To determine the error in the average count rate, write each count rate measurement in terms of total
counts observed per unit time. Assume that the error in the measurement time is negligible so that σti  0.
Then with the error propagation formula, the variance in the count rate is13
* & +2 & * +2 & * +2

N
∂ 
N N 
N N 
N N
σg2 = Gi ti 2
σ (Gj ) = 2
σ (Gi ) ti = Gi ti . (6.93)
j=1
∂Gi i=1 i=1 i=1 i=1 i=1 i=1

Now suppose that f (x) involves M different radiation source configurations and that multiple mea-
surements are made for each source configuration. Further, suppose f (x) takes sums and differences of
measurements for the different source configurations. For example, measurements are often taken with a ra-
dioisotopic source present and with the source removed to obtain background counts. Then the background
count rate is subtracted from the source count rate to obtain the net or background-corrected source count
rate. In general one seeks the average
 & 
M 
M 
Nm Nm
f (x) = (±)g m (Gm1 , . . . , GmNm , tm1 , . . . , tmNm ), = (±) Gmi tmi . (6.94)
m=1 m=1 i=1 i=1

Here Nm is the number of different measurements taken with the mth source configuration and Gmi and tmi
are the counts and count time for the ith measurement. From the error propagation formula, the variance
of this average is found to be ⎡
& * +2 ⎤
M 
Nm Nm
σf2 = ⎣ Gmi tmi ⎦ , (6.95)
m=1 i=1 i=1

from which the standard deviation σf is readily found.

%N
13 Alternatively, if N is greater than 10 or so, the sample variance s2 (g) = √ 1 − g)2 can be used to estimate σg2 .
N−1 i=1 (gi
Sec. 6.9. Error Propagation 225

Example 6.19: A scientist takes a 15-minute background measurement, resulting in B1 = 241. The
scientist then takes two radiation measurements of the sample, each over 10 minute periods, and observes
G1 = 1993 and G2 = 1957. During a third measurement, he is called to meeting, and stops the third
measurement at 6 minutes, recording G3 = 1165 counts. Before leaving, he removes the source and starts
a background measurement. When the scientist returns, the background measurement has continued for 67
minutes, yielding B2 = 1043 counts. What is the average net count rate and standard error?

Solution:
The net count rate is found by subtracting the background count rate from the gross count rate. From
Eq. (6.94), the net average count rate is
N =N  N =N 
 G G B  B

n= Gi tGi − Bi tBi , where NG = 3, NB = 2,


i=1 i=1 i=1 i=1

   
1993 cts + 1957 cts + 1165 cts 241 cts + 1043 cts
= − = 180.1 cpm.
10 min + 10 min + 6 min 15 min + 67 min
From Eq. (6.95), the variance is
⎡ = *N +2 ⎤ ⎡ N = *N +2 ⎤

NG
 G B B

σn = ⎣
2
Gi tGi ⎦ + ⎣ Bi tBi ⎦ , where NG = 3, NB = 2,
i=1 i=1 i=1 i=1

1993 cts + 1957 cts + 1165 cts 241 cts + 1043 cts
= + = 7.758 min−2
(10 min + 10 min + 6 min)2 (15 min + 67 min)2


The standard error is found to be σm = 7.758 = 2.785 min−1 . The net count rate and error are then
reported as 180.1 ± 2.79 cpm.

Equal Counting Times


If the count times are identical for the Nm measurements in each source configuration, i.e., tm1 = tm2 =
. . . = tmNm ≡ tm , then Eq. (6.92) reduces to,
* + * + * +
M
1 
Nm
Gmi M
1 
Nm M
1 
Nm
n= (±) = (±) gmi = (±) Gmi . (6.96)
m=1
Nm i=1 tm m=1
Nm i=1 m=1
Nm tm i=1

and the variance reduces to


⎡ +2 ⎤
  & * 
N
 & 

 
1 
M Nm Nm M m M Nm
2
σn = ⎣ Gmi tm ⎦ =
2
Gmi (Nm tm ) = gmi . (6.97)
2t
Nm
m=1 i=1 i=1 m=1 i=1 m=1 m i=1
226 Probability and Statistics for Radiation Counting Chap. 6

Example 6.20: A researcher takes a single radiation measurement on a sample in a low background
counting environment and observes G = 2310 counts in a one-minute counting period. Afterwards, the
researcher conducts a single one-hour long background measurement and observes B = 213 counts. What is
the net count rate and standard error?

Solution:
The net count rate is found by subtracting the background count rate from the gross count rate. From
Eq. (6.96), the net average count rate is,

1  Gi 1  Bi
NG NB
n= − , where NG = 1, NB = 1,
NG i=1 tG NB i=1 tB
 
G B 2310 cts 213 cts
= − = − = 2306.15 cpm.
tG tB 1 min 60 min
From Eq. (6.97), the standard error is
 1/2  1/2  1/2
G B g b 2310 cts 213 cts
σn = + = + = + = 48.06 cpm.
t2G t2B tg tb (1 min)2 (60 min)2
The count rate and error are reported to be 2306.15 ± 48.06 cpm.

Example 6.21: Before measuring a radioactive sample, a technician takes a 30-minute background mea-
surement, resulting in B1 = 513. The technician then takes four radiation measurements of the sample,
each over 5-minute measurement periods, and observes G1 = 2310, G2 = 2219, G3 = 2387, and G4 = 2264
counts. Afterwards, the technician conducts another 30-minute long background measurement and observes
B2 = 478 counts. What is the average net count rate and its standard error?

Solution:
The net count rate is found by subtracting the background count rate from the gross count rate. From
Eq. (6.96), net average count rate is (with NG = 4 and NB = 2)
   
1  Gi 1  Bi
NG NB
1 9180 cts 1 991 cts
n= − ,= − = 442.48 cpm.
NG i=1 tG NB i=1 tB 4 5 min 2 30 min

From Eq. (6.97), the standard error is


$ /1/2
1  Gi 1  Bi
NG NB
σn = 2
+ 2 , where NG = 4, NB = 2,
NG i=1 G
t2 NB i=1 t2B

"    #1/2
1 9180 cts 1 991 cts
= + = 4.82 cpm.
16 25 min2 4 900 min2
The count rate and error are reported to be 442.48 ± 4.82 cpm.
Sec. 6.10. Data Interpretation 227

6.9.7 Caution about Error Propagation


The error propagation formula of Eq. (6.75) is based on the assumption that the first two terms in the Taylor
series expansion for a function f (x1 , x2 , ..., xN ), evaluated at measured values x̂1 , x̂2 , . . . , x̂N , adequately de-
scribes its variation with the xi . The first two terms of the Taylor series expansion describe a linear variation
with the xi , and for radiation counting the function is evaluated about the mean of the data distribution.
Hence, for highly non-linear functions, such as high order polynomials and exponential functions, Eq. (6.75)
may not provide an adequate description. This discrepancy between the actual function and an estimate
from the truncated Taylor series expansion is especially of concern for arguments that are far from the mean
values (xi ).
Further, data are assumed to be independent and uncorrelated in Eq. (6.75). But there are situations
where this assumption is simply incorrect. For example, often a series of data is analyzed with linear
regression to determine a specific characteristic (or characteristics) of the underlying distribution. Examples
include the determination of a radioactive decay constant or a photon attenuation coefficient of a material.
From the least squares fit of the data, a slope and intercept are determined, and the data values actually are
correlated when determining these parameters. Under such situations, the covariance of the data may be an
important component of the standard error, hence it is advisable to actually use Eq. (6.74) in such cases.

6.10 Data Interpretation


In any statistical analysis where prediction or interpretation is drawn from a probability distribution function
lies the possibility of misinterpreting the data. For instance, in radiation counting, there is a possibility of
declaring a sample radioactive when in fact it is not, or the possibility of measuring a radioactive source,
but declaring it non-radioactive. Such concerns are especially important if the count rate from the suspected
radioactive source is comparable to that from background radiation. Consider a sample suspected of being
radioactive, with the hypothesis that the sample is not radioactive. This is termed the null hypothesis,
denoted by H0 . The other possibility is, of course, that the sample actually is radioactive, is termed the
alternative hypothesis, denoted Ha . If an experimenter measures the activity of the sample, then two following
possible errors in the interpretation of the data can occur [Devore 1991].
Type I error consists of rejecting the null hypothesis in favor of the alternative hypothesis Ha when in
fact H0 is true, meaning in this case declaring the sample radioactive when in fact it is not, termed a
false positive.
Type II error consists of accepting the null hypothesis H0 when it is incorrect, meaning the sample is
declared non-radioactive when it actually is radioactive, termed a false negative.
Such errors are difficult to identify, yet the probability of making either a Type I or Type II error can be
determined. The method used for determining these probabilities is referred to as “hypothesis testing.”14
The test procedure is usually defined by some measure called a test statistic or a rejection region. The
test statistic defines a quantity, whether it be the average value or some other statistic, with which the
observed data are to be interpreted. The rejection region is a range of values in which a new hypothesis is
accepted over the previous hypothesis. For radiation counting, one might use the average counts observed
from a calibration with the background radiation as a test statistic and the region greater than x + 2σ as
the rejection region. Hence, samples producing counts greater than x + 2σ are declared radioactive, and
samples producing counts below x + 2σ are deemed non-radioactive. Or, it may be hypothesized that a single
measurement is a good first estimate of the average number of counts expected per measurement, and the
rejection region is defined as some function of the standard deviation.

14 Although hypothesis testing is often used in probability and statistics, it is widely considered to be a branch of decision theory.
228 Probability and Statistics for Radiation Counting Chap. 6

Figure 6.19 shows the standard normal distribution in which the regions outside of z±1.96σ are designated
rejection regions. The remaining values of z are in the acceptance region. Given any hypothesis about the
distribution of Fig. 6.19, for instance the mean value, a measurement falling outside of z ± 1.96σ implies that
the hypothesis be rejected. The form shown in Fig. 6.19 is referred to as a two-tailed test because regions
on both sides of the mean value are designated as rejection regions. There are some circumstances in which
extreme values on only one side of the distribution is of interest. Such a test is referred to as a one-tailed
test.

Figure 6.19. The standard normal distribution showing the rejection region
and the acceptance region. The sum of the shaded regions represents 5% of the
normal distribution, and the light region represents 95% of the distribution.
There is a 95% chance that the next measurement results in z falling within
the acceptance region and only a 5% chance that the next measurement results
in z falling in either of the shaded regions.

Example 6.22: Suppose a single radiation measurement is performed in which x̂ = 194 counts are
observed. Such counts follow a Gaussian√distribution. The hypothesis H0 is declared that 194 is the mean
value with the standard deviation σ = x̂ = 13.93. Hence, the mean value is the test statistic. It is also
asserted that the hypothesis is rejected should the next independent measurement produce a count outside
of ±1.96σ (the rejection region—see the shaded area in Fig. 6.20). The rejection region is 5% of the area
under the Gaussian PDF, whereas the acceptance region is 95% of the area.
Should the next measurement produce a count that falls in the shaded area of Fig. 6.20, then the
hypothesis H0 is rejected at a 0.05 level of significance. For instance, if another measurement produced
121 counts, then at the 0.05 level, the hypothesis that 194 is the mean value of the underlying Gaussian
distribution would be rejected. What this also means is, because 5% of the PDF lies outside of ±1.96σ, then
there is a 5% probability that the experimenter can make a Type I error by declaring the mean is not 194
when it actually is!
Sec. 6.10. Data Interpretation 229

Figure 6.20. The Gaussian


√ distribution fN (x|x̄, x̄) as predicted for the case in which
it is assumed that x = σ = 194. The sum of the shaded regions represent 5% of the
Gaussian PDF, and the light region represents 95% of the PDF.

6.10.1 Radiation Detection Limits


Sometimes a suspected radioactive sample produces counts similar to those of a background count for the
same counting time. How is it possible to determine if the sample is actually radioactive or not? Clearly
such a case involves Types I and II errors.
As shown in Fig. 6.21, the Gaussian background and radioactive sample distributions of counts can
overlap. In this plot the expected background counts are subtracted from both the background and sample
count distribution, i.e., the Gaussian distributions are plotted as a function of the net counts. Because the
two distributions overlap it is possible an experimenter can declare a sample radioactive, when it is not
(Type I error), or declare the sample “clean” when it is actually radioactive (Type II error).
The net sample counts are defined the gross sample counts G less the background counts B, i.e., Ns =
G − B. The standard deviation of the background is σB , and the standard deviation of the total counts from
the sample is σG . If the sample is not radioactive (Ns  0), then it is expected that G − B  B − B  0.
Under such a condition, the standard deviation is

σ(Nnet ) ≡ σ0 = 2 + σ2 =
σB B
2 =
2σB 2B. (6.98)

But should the sample produces net counts comparable to that of the background (Ns  B or G  2B), the
standard deviation is approximately,
√ √ √
σ(Nnet )  G + B = 2B + B = 3B. (6.99)
230 Probability and Statistics for Radiation Counting Chap. 6

The concepts of Type I and Type II error are important for radiation counting in the presence of significant
background radiation. Typically the limiting ability to detect non-background radiation is given by the
minimum detectable activity (MDA), which defines the minimal amount of radiation that can be detected
given a specific confidence limit defined by the rejection region and radiation background [Currie 1968;
Rucker 1995].15
Related to the MDA is the critical detection limit (CDL), which defines the limit by which counts from
a sample can be reported with a preset rejection region. Hence, any measurement resulting in counts below
the CDL is not worth reporting, based on a one-tailed test at the low end of the sample measurement count
distribution. The CDL is defined by the confidence limit defined by some fixed multiple of the standard
deviation of the sample distribution.
Shown in Fig. 6.22 are two net count distributions for background and sample measurements in which the
tails of the distributions overlap. It should be remembered that the background influences the MDA, and the
MDA is determined by the error that an experimenter deems as tolerable. Hence, given some predetermined
test and rejection regions, the adjacent shaded regions α and β can be defined, in which α represents the
probability of making a Type I error and β represents the probability of making a Type II error. The decision
to state that a sample is not radioactive is defined by 1 − α, in which α = kα σ0 , is a fraction of the high-end
tail of the Gaussian background distribution, where values of kσ are listed in Table 6.6. For instance, it is
quite common to choose kα = 1.645 so that α = 0.05 and that 1 − α = 1 − 1.645σB = 0.95. Because the
background net count distribution is centered about zero, the CDL (denoted as LC ) is

LC = kα σ0 = kα 2B. (6.100)

Hence, a sample measurement producing net counts below the CDL is declared non-radioactive. The
MDA must be larger than CDL and can be defined in terms of the CDL by setting the MDA equal to the
CDL plus some confidence interval with an overlapping rejection region defined in Fig. 6.22 as β. Hence, the
MDA, denoted by LD , is
LD = LC + kβ σN = kα σ0 + kβ σNs . (6.101)
Typically, β is chosen to be 0.05, hence kβ = kα = 1.645.
Two limiting cases in which the sample yields low counts are now considered. In the first case, assume
that the background and net sample count rates are similar.
CASE 1: (Ns  B) .
√ √ √ √
LD = kα σB + kβ σN = kα 2B + kβ G + B = kα 2B + kβ 3B
√ √
= 1.645( 2σB + 3σB ) = 5.176σB . (6.102)
Suppose, however, the net sample counts are quite a bit smaller than those of the background radiation.
With the same criteria for kβ and kα , the following is stated,
CASE 2: (N  B). The MDA can be rewritten as

LD = LC + kβ σN = LC + kβ LD + σ02 , (6.103)
which, when combined with Eq. (6.100), and solved for LD yields
 < 
kβ2 4LC 4L2C
LD = LC + 1+ 1+ 2 + 2 2 . (6.104)
2 kβ kα kβ

15 Theuse of the word “activity” in the MDA is unfortunate because the MDA does not refer to the true activity of a sample
(number of decays per unit time), but rather to the number of counts produced above background.
Sec. 6.10. Data Interpretation 231

Figure 6.21. Overlapping Gaussian distributions for a case in which a


radioactive sample produces comparable counts as does the background ra-
diation. Here the background counts have been subtracted from both distri-
butions and are thus plotted as a function of the net counts, i.e., background
subtracted counts or net counts. In this hypothetical case, the background
B = 25 so that an average net measurement for a non-radioactive sample is
0 counts. The low-level radioactive sample has Ns = 25 counts. Notice the
significant overlap between the two distributions, hence leaving considerable
room for misinterpretation of the radioactive nature of the sample.

Figure 6.22. Overlapping Gaussian distributions for a case in which a


radioactive sample produces a net count comparable to that of the back-
ground radiation. The area of the shaded region α is the probability of a
Type I error, and the area of the shaded region β is the probability of a
Type II error.
232 Probability and Statistics for Radiation Counting Chap. 6

If kα = kβ = k, then the above reduces to [Currie 1968],

LD = k 2 + 2LC , (6.105)

a commonly used test for low level radiation. Hence, a sample measurement with net counts above the MDA
is declared radioactive with 95% confidence.

Example 6.23: A nuclear engineering student discovers an advertisement for “radioactive marbles” on the
internet and decides to purchase a few for his collection of atomic memorabilia. Upon receiving the yellowish-
green marbles, the student decides to take a measurement to determine if the marbles really are radioactive.
A 95% confidence level is decided upon for both Types I and II error, so that k = kα = kβ = 1.645. The
following data are collected: G = 217 counts, B = 194 counts, and Ns = 217 − 194 = 23 counts. Then

LD = k2 + 2LC = k2 + 2k 2B
√ √
= (1.645)2 + 1.645(2) 2 194 = 2.706 + 4.65(13.93) = 67.3.

This result indicates that at least 67.3 net counts should be observed from the sample to reduce the prob-
ability of a Type II error to only 5%. With the MDA at 67.3, but Ns = 23, the student suspects that the
marbles are not radioactive. The CDL is found to be
√ √
LC = kα σ0 = kα 2B = (1.645) 2(13.93) = 32.4.

Since Ns < LC , the result is considered “not worth reporting,” and the student determines with 95%
confidence that the marbles are not radioactive. (Next time, buy the red Fiesta Ware!)

In recent years, the standard that defined the use of MDA and CDL was updated to address perceived
deficiencies [Strom, 2001; ANSI 13.30, 2011]. Measurements and analysis indicate that Eq. (6.100) routinely
overestimates the fraction of false positive events [Strom, 2001], becoming large as α is reduced (α ≤ 0.05).
The inaccuracy stems from the fact that a Gaussian distribution is assumed for these low count rates, when
in fact the actual average and variance for the observed counts are not well defined.
An alternative, but equivalent, expression for Eq. (6.100) that incorporates varying count rates is [Nichol-
son 1963], <  
B 1 1
LC (Rn , α) = kα + , (6.106)
tB tB tG
where tB is the background count time and tG is the gross count time, and LC is given as a count rate.
Eq. (6.106) is a function of the net count rate Rn and α, whereas Eq. (6.100) is a function of the observed net
counts and α. One suggested method of correction is to substitute (B + 1) for B in the analysis [Strom 2001],
which implies that the actual average background count observed (or predicted with a Gaussian model) is
higher than the measured average. The correction is based on the “belief” that the observations can be
described by a uniform Bayesian probability distribution function where the expected value of the observed
background counts is B + 1. Substitution for B yields,
<  
(B + 1) 1 1
LC (Rn , α) = kα + , (6.107)
tB tB tG
Sec. 6.10. Data Interpretation 233

where LC is given as a count rate. Although Eq. (6.107) reduces the frequency of false positives from
Eq. (6.100), the estimated false positive rate is still higher than the actual rate.
Alternative treatments for LC are listed and briefly described in the literature [Strom 2001]. The study
compares eight different decision rules in which it was concluded that all of the methods introduce bias
into the predicted false positive rate, with Eq. (6.100) yielding the highest false positive rate. Eq. (6.107)
adequately suppresses the false positive rate; however, alternative methods appear to yield even lower false
positive rates, but apparently risk an increase in false negatives for low counting rates.

6.10.2 Chi-Square Test for “Goodness” of Data


Data accumulated by a counting system may yield results that are affected by systematic errors. For instance,
electronic noise may be a source of significant problems, especially if the lower level discriminator (LLD)
is set too low. It is often important that an experimenter test the counting system for such possible issues
before beginning a radiation measurement experiment.
In Section 6.8 it was shown that counting statistics can be modeled with a Gaussian PDF with mean μ
and variance σ2 = μ, provided that the probability p of observing a decay is small and the sample mean x is
larger than approximately 25. Therefore, given a set of measurements x̂1 , x̂2 , . . . , x̂N , it should be possible
to compare in some way the population variance σ 2 to the sample variance s2 of Eq. (6.26). One approach
is to calculate the χ2 statistic defined as16
%N
i=1 (xi − μ)2
χ ≡
2
, (6.108)
σ 2 (x)

where xi is the ith random sample from N (x|μ, σ). Here χ2 is a random variable and is distributed according
to the χ2 PDF [Mood et al. 1974]

1 2
f (χ2 |ν) = (χ2 )(ν/2)−1 e−χ /2
, x > 0, (6.109)
2ν/2 Γ(ν/2)

with ν = N degrees of freedom. This PDF is illustrated in Fig. 6.23 for ν = 1, 2, 3, 4, and 5. From this
figure this distribution is seen to be asymmetrical about the mean, although the χ2 distribution becomes
increasingly symmetric as ν becomes large.
How might χ2 help one to decide if a counting system is operating properly? If one were to estimate μ
by x and use the measured x̂i in place of the xi then, with Eq. (6.26), χ2 would be estimated as
%N
i=1 (x̂i − x)2 (N − 1)s2
χ̂ ≡
2
= . (6.110)
σ2 σ2

Divide by (N − 1) to obtain the so-called reduced chi-square statistic χ2ν = s2 /σ 2 . Thus, if the data are a
good fit to the Gaussian model, then χ2ν should be close to unity. If, however, s2 is greatly different from
σ 2 , then χ2ν would be either very small or much greater than unity, an indication that something is probably
amiss with the counting system. Calculation of the reduced χ2ν is a very easy and quick way to check a
counting system.
Although the above reduced chi-squared procedure is a quick and easy method, it does not yield any
quantification of the confidence one has about how well the data fit the Gaussian model. The chi-squared
test for “goodness” of data, begins by calculating a measured or critical χ2 value from Eq. (6.108), with the

16 The square on χ2 is to remind one that this statistic can never be negative.
234 Probability and Statistics for Radiation Counting Chap. 6








  


 




            

Figure 6.23. The χ2 probability distribution function for ν = 1, 2, 3, 4, and 5.

observed data, i.e., μ  x and σ 2  x, as

1
N
2 =
χ (x̂i − x)2 . (6.111)
x i=1

This statistic is also distributed as the χ2 PDF but now with N − 1 degrees of freedom because μ has been
approximated by x (see Section 6.5.4).
The probability α of observing a χ2 greater than χ2α is
 ∞
1 2
α(ν) = ν/2 Γ(ν/2)
(χ2 )(ν/2)−1 e−χ /2 dχ2 . (6.112)
2
χα 2

For example, shown in Fig. 6.24 is the χ2 distribution for ν = 20, in which the shaded region defines the
probability of observing a χ 2 value between the limits χ2α = 27 and ∞.
2
Given any χα and ν, the probability α(ν) of obtaining a value of χ 2 greater that χ2α can be found by
numerical evaluation of Eq. (6.112). Conversely, (1 − α(ν)) is the probability of obtaining a χ 2 less than
χα . Figure 6.25 shows values of α for ν = 1, 2, 3, 4, and 5 as a function of the critical value χ2α . Shown
2

in Table 6.8 are the values χ2α , with the associated probabilities α, for ν ranging from 1 to 30. Thus, the
chi-square goodness-of-fit test consists of calculating χ 2 from the measured data. Then from Table 6.8 find
the probabilities of obtaining a value larger or smaller than χ 2 . If either of these probabilities is much greater
or much less than 0.5, then the data are suspect.
Typically, an experimenter should choose a confidence interval to determine whether or not the observed
data are unusual. For instance, if a χ 2 value for a set of N measurements yields an α of 0.05, then there is
only a 5% probability of observing a higher value should a new data set of N measurements be acquired.
Similarly, should the χ2 value yield α of 0.95, there is a 95% probability that the next set of N measurements
produces a higher value. In either case, the result is at the extremes of the χ2 distribution, a strong indication
Sec. 6.10. Data Interpretation 235

Figure 6.24. The χ2 probability distribution function for ν = 20, showing a


critical value of χ2α = 27, where α is the shaded region.




  






 
 

            


Figure 6.25. The values of α for ν = 1, 2, 3, 4, and 5 as a function of various
critical values of χ2 .

that the data are not following the expected Gaussian model. An acceptable confidence interval should be
decided upon by the experimenter that minimizes either Type I or Type II error, depending on which is
more important in the data analysis.
236 Probability and Statistics for Radiation Counting Chap. 6

Example 6.24: An experimenter takes a series of five measurements with a counting system to test the
>2
goodness of the data and obtains the following counts: 302, 311, 297, 307, and 299. Find the value of χ
2
 .
and determine the probability of observing a value greater than (or less than) χ

Solution:
From Eq. (6.111),
%N
2 (x − xi )2 1.44 + 60.84 + 38.44 + 14.44 + 17.64
 =
χ i=1
= = 0.438.
x 303.2
From Table 6.8 with ν = 5 − 1 = 4, the value of χ 2 = 0.438 falls between 0.297 and 0.484 under the
probability columns (α) of 0.99 and 0.975, respectively. Application of linear interpolation between these
χ2α values, α is found to be 0.9787. This result means that a new series of measurements would have a
97.87% chance of having a χ 2 value greater than 0.438 (or a 2.13% of observing a value less than 0.438).
The experimenter should be suspicious of the data!
What do these results mean? Because the distribution yields a low value for χ2 , the variance about the
mean is much smaller than should be observed for samples from a Gaussian distribution. Had the χ 2 value
been relatively large, for instance near 14 for the case with ν = 4, then the variance about the mean is much
larger than should be observed for a Gaussian distribution. Finally, a χ 2 value yielding α ≈ 0.5 describes
the expected variance for a Gaussian distribution.

The χ2 test is an important tool. If the value of the probability α falls far from 0.5, then something may
be wrong with the detector, the electronics, or the counting system arrangement. Possible sources of the
problem include:

1. The lower level discriminator (LLD) is set too low, hence the electronic noise is being measured as a
significant addition to the real radiation counts.

2. Pickup from ground loops and other electronic noise.

3. Poor preparation of the radioactive sample.

4. Faulty equipment or malfunctioning equipment.

Finally, the experimenter must decide if the result of the chi-squared test is simply a matter of statistics.
Because the χ2 distribution has a range [0,∞], all positive values of χ2 are possible. Hence, the observation
of a single χ value yielding an extreme value of α is not alarming, and might be considered an outlier.
2

However, if several subsequent tests also produce χ 2 values with extreme values of α, then it is almost
certain that a problem exists with the counting system.

6.10.3 Presentation of Data


Presentation of counting data should also give the estimated one-sigma errors. In plots of counting data
error bars are typically used to show the experimental error associated with each data marker. The length
of the error bars are scaled to properly depict the values of ±σ. If the error is too small to be properly
represented by error bars, then the data are represented only by the data markers. In some cases, error bars
should be shown along both the ordinate and abscissa of a Cartesian graph.
Theoretical plots, empirical plots and curve fitting routines are depicted by a continuous smooth curve
without data points. With plotting software, an experimenter may be tempted to use data points and a
Table 6.8. Critical Values for the χ2α Distribution.
PP
0.995 0.99 0.975 0.95 0.90 0.75 0.50 0.25 0.10 0.05 0.025 0.01 0.005
ν
PPα
P
1 0.000 0.000 0.001 0.004 0.016 0.102 0.455 1.323 2.706 3.843 5.025 6.637 7.882
2 0.010 0.020 0.051 0.103 0.211 0.575 1.386 2.773 4.605 5.992 7.378 9.210 10.597
Sec. 6.10. Data Interpretation

3 0.072 0.115 0.216 0.352 0.584 1.213 2.366 4.108 6.251 7.815 9.348 11.344 12.837
4 0.207 0.297 0.484 0.711 1.064 1.923 3.357 5.385 7.779 9.488 11.143 13.277 14.860
5 0.412 0.554 0.831 1.145 1.610 2.675 4.351 6.626 9.236 11.070 12.832 15.085 16.748
6 0.676 0.872 1.237 1.635 2.204 3.455 5.348 7.841 10.645 12.592 14.440 16.812 18.548
7 0.989 1.239 1.690 2.167 2.833 4.255 6.346 9.037 12.017 14.067 16.012 18.474 20.276
8 1.344 1.646 2.180 2.733 3.490 5.071 7.344 10.219 13.362 15.507 17.534 20.090 21.954
9 1.735 2.088 2.700 3.325 4.168 5.899 8.343 11.389 14.684 16.919 19.022 21.665 23.587
10 2.156 2.558 3.247 3.940 4.865 6.737 9.342 12.549 15.987 18.307 20.483 23.209 25.188
11 2.603 3.053 3.816 4.575 5.578 7.584 10.341 13.701 17.275 19.675 21.920 24.725 26.757
12 3.074 3.571 4.404 5.226 6.304 8.438 11.340 14.845 18.549 21.026 23.337 26.217 28.300
13 3.565 4.107 5.009 5.892 7.042 9.299 12.340 15.984 19.812 22.362 24.736 27.688 29.819
14 4.075 4.660 5.629 6.571 7.790 10.165 13.339 17.117 21.064 23.685 26.119 29.141 31.319
15 4.601 5.229 6.262 7.261 8.547 11.037 14.339 18.245 22.307 24.996 27.488 30.578 32.801
16 5.142 5.812 6.908 7.962 9.312 11.912 15.339 19.369 23.542 26.296 28.845 32.000 34.267
17 5.697 6.408 7.564 8.672 10.085 12.792 16.338 20.489 24.769 27.587 30.191 33.409 35.718
18 6.265 7.015 8.231 9.390 10.865 13.675 17.338 21.605 25.989 28.869 31.526 34.805 37.156
19 6.844 7.633 8.907 10.117 11.651 14.562 18.338 22.718 27.204 30.144 32.852 36.191 38.582
20 7.434 8.260 9.591 10.851 12.443 15.452 19.337 23.828 28.412 31.410 34.170 37.566 39.997
21 8.034 8.897 10.283 11.591 13.240 16.344 20.337 24.935 29.615 32.671 35.479 38.932 41.401
22 8.643 9.542 10.982 12.338 14.041 17.240 21.337 26.039 30.813 33.924 36.781 40.289 42.796
23 9.260 10.196 11.689 13.091 14.848 18.137 22.337 27.141 32.007 35.172 38.076 41.638 44.181
24 9.886 10.856 12.401 13.848 15.659 19.037 23.337 28.241 33.196 36.415 39.364 42.980 45.559
25 10.520 11.524 13.120 14.611 16.473 19.939 24.337 29.339 34.382 37.652 40.646 44.314 46.928
26 11.160 12.198 13.844 15.379 17.292 20.843 25.336 30.435 35.563 38.885 41.923 45.642 48.290
27 11.808 12.879 14.573 16.151 18.114 21.749 26.336 31.528 36.741 40.113 43.195 46.963 49.645
28 12.461 13.565 15.308 16.928 18.939 22.657 27.336 32.620 37.916 41.337 44.461 48.278 50.993
29 13.121 14.256 16.047 17.708 19.768 23.567 28.336 33.711 39.087 42.557 45.722 49.588 52.336
30 13.787 14.953 16.791 18.493 20.599 24.478 29.336 34.800 40.256 43.773 46.979 50.892 53.672
40 20.707 22.164 24.433 26.509 29.051 33.660 39.335 45.616 51.805 55.759 59.342 63.691 66.766
50 27.991 29.707 32.357 34.764 37.689 42.942 49.335 56.334 63.167 67.505 71.420 76.154 79.490
60 35.535 37.485 40.482 43.188 46.459 52.294 59.335 66.981 74.397 79.082 83.298 88.379 91.952
70 43.275 45.442 48.758 51.739 55.329 61.698 69.334 77.577 85.527 90.531 95.023 100.425 104.215
80 51.172 53.540 57.153 60.392 64.278 71.145 79.334 88.130 96.578 101.879 106.629 112.329 116.321
90 59.196 61.754 65.647 69.126 73.291 80.625 89.334 98.650 107.565 113.145 118.136 124.116 128.299
100 67.328 70.065 74.222 77.930 82.358 90.133 99.334 109.141 118.498 124.342 129.561 135.807 140.169
237
238 Probability and Statistics for Radiation Counting Chap. 6

dot-to-dot line linking the calculated or theoretical values; but this is simply incorrect. In plotting data a
clear distinction must always be made between experimental data points and a theoretical comparison (or
curve fit to the data).
Shown in Fig. 6.26 is a counting curve for a proportional gas-filled radiation counter17 versus the high
voltage applied to operate the detector. The curve shows the counts observed and the standard error (±σ)
for each measurement. In this example, the uncertainties in the applied voltage were deemed to be smaller
than the data markers and, hence, horizontal error bars are omitted. Also in the graph a curve fitted line
is drawn freehand through the data. Such a curve does not represent a theoretical or empirical equation.
Equivalently, bicubic splines, for example, can be used to produce a smooth curve through the data [Press
et al. 1992]. However, such a line is not necessary, but is usually provided to show the trend of the data
for presentation purposes. Notice that the trend line is not drawn through each data point, but rather is a
smooth representation, showing an estimated average of the data. Error bars are present on data markers
in which the value of ±σ exceeds the marker size.
Fig. 6.27 depicts data and a theoretical comparison for an experiment in which different thicknesses
of a Cu attenuator are placed between a detector and a 137 Cs source. As the Cu thickness is increased,
the gamma rays passing through the Cu sheet and entering the detector are exponentially reduced. The
example shows the theoretical variation with Cu thickness, for a specific detector and source strength, to
be 300 counts when no attenuator is present. Also shown are the theoretical limits ±σ for the attenuated
counts based on Gaussian counting statistics. The actual data observed are presented as data markers with
error bars defined by ±σ for each data point. Finally two Gaussian distributions show how data samples at
two Cu thicknesses should be distributed.
Fig. 6.27 also reveals another important aspect of data presentation, namely it is statistically expected
that only 68.3% of the error bars should actually come into contact with the true mean value. In other
words, for data following a Gaussian PDF, 31.7% of the data markers and accompanying error bars should
not contact either the theoretical or sample mean! Hence, it is simply incorrect to connect all experimental
data points together by lines drawn between each pair of data markers.

6.10.4 Concluding Remarks


Radiation emissions are stochastic (non-deterministic) such that the observation of a radioactive decay event
cannot be predicted exactly; rather only probability statements can be made of observing an event within a
specified period of time. A true mean value (population mean) of the radioactive decay rate can be calculated
from the decay constant of the radionuclide, and the probability of observing a radioactive decay is bounded
by the variance about that mean. However, experimenters, who do not know the decay constant, must use
measured values to obtain the sample mean and sample variance. Almost always there is a difference between
the true and sample means, and a difference between the population sample variances. These differences
generally become smaller as more data are accumulated.
Three basic statistical models are developed that can describe radioactive decay and counting statistics
with the Gaussian (or normal) distribution most often used for radiation counting. Many examples are
included to assist in understanding the use of these models. The reader is warned that the models apply
only to stochastic processes, and do not account for systematic and sampling errors. Systematic errors may
be introduced by biases unknown to the experimenter, such as malfunctioning equipment. The χ-square
test can often expose that such biases exist. Sampling errors arise from performing measurements on a
sample population different from the one desired. For example, a radioactive sample containing two types of
radionuclides or a background count with the radioactive sample not sufficiently far away from the detector
would cause sampling errors.

17 Proportional counters, a type of gas-filled detector, are covered in Chapter 10.


Sec. 6.10. Data Interpretation 239




  


         
  

Figure 6.26. Example of data points with error bars, showing a


counting curve for a gas-filled proportional counter and a smooth
curve fit through the data.



  !
 

%! ! # &


 !&   !
  


   !"! !

# $! 



          

  
Figure 6.27. Example of data points with error bars, showing the
true mean and standard deviation, along with experimental standard
deviations for each data point.

The purpose of this chapter is to provide the necessary tools for an experimenter to perform basic
radiation measurements. Throughout this book other more specialized statistical models used in radiation
detection are introduced. There are also a huge number of other statistical models used in other branches
of science and engineering that are not discussed here. For details on these other probability and statistical
models for engineering and science, and their proper application, the reader is directed to the reference list
at the end of the chapter.
240 Probability and Statistics for Radiation Counting Chap. 6

PROBLEMS
1. What is the probability of tossing heads 10 times out of 15 with a “fair” coin?

2. “Introduction to Engineering Concepts 101” is a huge class with 375 students enrolled. Use Poisson
statistics to determine the probability that exactly 3 students in the class have a birthday today. Plot
the probability distribution function for 0 through 10 students having birthdays.

3. An amateur archer practices once every afternoon, shooting 100 arrows and, generally, hits the target.
One time out of 15, the archer hits the bull’s eye. After shooting 100 arrows, what is the average number
of bull’s eyes achieved, and what is the standard deviation? What is the probability that the archer
strikes exactly 10 bull’s eyes after 100 tries?

4. A set of radiation measurements is made with the following results:

54, 89, 64, 102, 90, 78, 56, 74, 88, 42,
70, 94, 50, 82, 100, 64, 72, 78, 58, 76

Find the sample mean, variance and standard deviation.

5. Ten radiation measurements are conducted from which a standard error is determined. If an eleventh
measurement is conducted under identical conditions, by what amount does the standard deviation
change?

6. ACME Roadrunner Company manufactures alternators with a one-year guarantee. Random sampling
of alternators yielded the following number of months to failure for 22 alternators:

37, 25, 44, 51, 26, 41, 18, 29, 58, 34, 43
31, 11, 27, 40, 39, 52, 23, 36, 38, 45, 55

Determine the experimental mean, median and variance of the data distribution. Find the 10% trimmed
mean and compare it to the median. Use a Gaussian PDF to estimate what percentage of alternators
fail and must be returned for a warranty replacement?

7. Show that Eq. (6.95) reduces to


1
2N  
12
3
 Gi Bi
σn = + 2
N i=1 t2Gi tBi

if the number of measurements performed N is the same for both gross and background counts, with
all tG equal and all tB equal.

8. A measurement is conducted with 662 keV gamma rays from a 137 Cs source. A detection system
records an average counting rate of 125 cpm. A background measurement records an average count
rate of 15 cpm. If a 30-minute background measurement is performed, how long must the 137 Cs source
measurement be in order to reduce the standard error of the net counts below 1%?

9. A radiation measurement is conducted in which a total gross number of counts is 2109, taken over 1
minute. A 10-minute background measurement is taken, resulting in 312 counts. What is the net count
rate and standard deviation (in counts and in percent)?
Problems 241

10. The following set of measurements, each for a six-second duration, resulted in the following number of
counts:

70, 64, 49, 58, 57, 52, 59, 53, 53, 58, 63, 61, 62, 68, 67, 51, 56, 54, 51, 66
66, 68, 71, 67, 51, 64, 73, 58, 69, 62, 56, 60, 57, 53, 57, 52, 55, 65, 61, 58
56, 61, 55, 70, 65, 68, 73, 57, 62, 58, 55, 63, 54, 58, 57, 64, 58, 66, 54, 49
68, 54, 62, 58, 79, 74, 53, 63, 58, 51, 56, 60, 56, 57, 62, 62, 59, 50, 63, 57
72, 45, 57, 47, 48, 62, 59, 53, 40, 77, 79, 48, 51, 69, 65, 60, 58, 71, 64, 48

(a) Calculate the sample mean, sample variance and the sample standard deviation. (b) Plot the data
distribution function and indicate the mean and standard deviation. (c) Use the sample mean to plot the
expected Gaussian PDF on the same graph. (d) Compare the experimental and theoretical distributions
by examining the variances and standard deviations.

11. A measurement is conducted with a 356-keV gamma-ray source that produces 1267 counts in a period
of 5 minutes. A 2-mm thick sheet of material is placed between the source and the detector and the
detector records 874 counts in 5 minutes? What is the attenuation coefficient and its standard error for
the material?

12. The following measurements were taken over five-minute periods each:

1288, 1443, 1377, 1341

and the following background measurements were taken over ten-minute periods each:

351, 436, 379, 414

Calculate the net counting rate per minute and the associated percent error.

13. A measurement was taken over a period of five minutes, resulting in 1417 counts. The background was
measured for one hour, resulting in 315 counts.

1. What is the average counting rate per minute and its percent standard error?
2. What is the estimated number of counts and its percent standard error for a one-hour measurement?
3. Use the average cpm to find the percent standard error if the measurement was conducted for one
hour as opposed to five minutes. How does this result compare to the five-minute measurement?

14. Prove that the covariance (xi − xi )(xj − xj ) can be approximated by xi xj  − xi xj . [Hint: Start by
expanding (xi − xi )(xj − xj )].

15. The half-life of a radiation source is sought. The first measurement, taken over a period of 1 minute,
yielded 2350 counts. Ten minutes later, a second measurement was started, again over a 1-minute period,
and yielded 1780 counts. What is the half-life of the source and the standard error in the measured
half-life?

16. Perform the χ2 test on the data of Example 6.7. If a new set of measurements is taken under identical
2 value is greater? What is your determination of the
conditions, what is the probability that the new χ
“goodness” of the data?
242 Probability and Statistics for Radiation Counting Chap. 6

17. Use the reduced chi-squared statistic to examine the “goodness” of the data in Example 6.7.

18. Derive Eq. (6.104) using the results of Eq. (6.100) and Eq. (6.101). Show that if kα = kβ , then Eq. (6.104)
reduces to Eq. (6.105).

19. An unmarked sample was found on the bottom shelf, way in the back, of the neutron activation analysis
(NAA) lab. It is unknown how old this sample is, and unfortunately, whether or not it is still radioactive.
The background recorded by a counting system in the NAA lab is 35 cpm. For a one-minute measure-
ment, what is the CDL required to produce with 95% confidence that the sample is not radioactive?
What is the MDA required for 95% confidence that the sample is still radioactive? Repeat your analysis
for a 60-minute measurement.

20. You are a final contestant on the Let’s Make a Deal! show, and must pick one of three doors, behind
which only one door has the grand prize, and behind the other two doors there is a pallet of dog food.
After making your initial selection, one of the doors that you did not choose is opened to reveal a pallet
of dog food, hence either the door you picked or the remaining closed door has the grand prize. You
are then given the opportunity to change your choice to the other closed door. Should you make the
change? Determine the statistics of winning if you change as opposed to keeping your original choice.

REFERENCES
ANSI 30.13, “Performance Criteria for Radiobioassay, An Ameri- MOOD, A.M., F.A. GRAYBILL, AND D.C. BOES, Introduction to
can National Standard,” Health Physics Society, American Na- the Theory of Statistics, 3rd Ed., New York: McGraw-Hill,
tional Standards Institute, ANSI/HPS N13.30-2011, 2011. 1974.
BEVINGTON, P.R. AND D.K. ROBINSON, Data Reduction and Er- NICHOLSON, W.L., Fixed Time Estimation of Counting Rates
ror Analysis for the Physical Sciences, 2nd Ed., New York: with Background Corrections, AEC R and D Report HW-76279,
McGraw-Hill, 1992. Richland, WA: Hanford Works, 1963.
BOX, G.E.P., W.G. HUNTER, AND J.S. HUNTER, Statistics for Ex- PRESS, W.H., B.P. FLANNERY, S.A. TEUKOLSKY, AND W.T.
perimenters, New York: Wiley, 1978. VETTERLING, Numerical Recipes, Cambridge, UK: Cambridge
University Press, 1986.
CRAMÈR, H., Mathematical Methods of Statistics, Princeton, NJ:
Princeton Univ. Press, 1946. RUCKER, T.L., “Methodologies for the Practical Determination
and Use of Method Detection Limits,” J. Radioanalytical and
CURRIE, L.A., “Limits for Qualitative Detection and Quantitative Nuclear Chemistry, Articles, 192, 345–350, 1995.
Determination,” Analytical Chemistry, 40, 586–593, 1968.
STROM, D.J. AND J.A. MACLELLAN, “Evaluation of Eight Decision
DEVORE, J.A., Probability and Statistics for Engineering and the Rules for Low-Level Radioactivity Counting,” Health Physics,
Sciences, 3rd Ed., Pacific Grove: Brooks-Cole, 1991. 81, 27–34, 2001.
KENDALL, M. AND A. STUART, The Advanced Theory of Statis- TAYLOR, J.R., An Introduction to Error Analysis, 2nd Ed., Mill
tics, 4th ed., Vol. 1, New York: MacMillan Publishing, 1977. Valley: University Science, 1997.
Chapter 7

Source and Detector Effects in


Radiation Measurements

An experiment is a question which science poses to Nature,


and a measurement is the recording of Nature’s answer.
Max Planck

The purpose of making radiation measurements is usually to infer information about the source of the
radiation. In particular, a detector response, such as a count rate, is often used to estimate the strength
or intensity of the radiation particles emitted by a source. Typically, the emission rate of a specified type
of radiation is sought. Although the detector count rate is approximately proportional to the emission rate
of the radiation from the source, there are many correction factors (some small, some large) that must be
made to the observed count rate to obtain an accurate estimate of the source strength. For example, not all
emitted radiation is emitted in a direction that intersects the detector volume. Likewise radiation emitted
toward the detector can be scattered by the surrounding medium into directions pointing away from the
detector. Thus, to accurately infer information about source strengths it is important to understand how
the source strength is related to the detector’s response. The several effects that must be accounted for are
the topics of this chapter.
To limit the scope of this chapter, the sources of radiation considered in this chapter are assumed
to be radioactive sources which emit radiation isotropically. Other sources of radiation such as cosmic
rays, accelerator sources, radiation from reactor beam ports, x-ray machines, etc., have their own special
phenomena that must be considered to infer accurate source strengths.

7.1 Detector Efficiency


Upon the detection of radiation, a proper calculation of the source activity, or radiation field, requires an
understanding of the detector response in the local environment. The ability of a detector to respond to
radiation is often reported as “efficiency”, yet there are multiple definitions for detector efficiency, which
include absolute efficiency, relative efficiency, and intrinsic efficiency [McGregor and Shultis 2011].
Absolute efficiency A is defined as the ratio of the measured number of counts recorded by the detector
to the total number of emissions from the radiation source during a time Δt, or, equivalently, the ratio of
the count rate Rdet to the source emission rate,
Rdet
A = n , (7.1)
AB i=1 Ci

where A is the source activity, B is the branching ratio or the probability, per radioactive decay, of emission
of the radiation of interest and Ci are various correction factors that apply to the measurement. A significant
characteristic of absolute efficiency measurements is that they are sensitive to changes in the source/detector

243
244 Source and Detector Effects Chap. 7

geometry. Hence, reporting the absolute efficiency is of little value unless the experimental arrangement
is described with adequate specificity to permit accurate reproduction of the measurement. The absolute
efficiency depends critically on the detector’s performance characteristics and on the geometrical positioning
of the detector with respect to the radiation source. There are conditions under which absolute efficiency is a
standard for reporting a detector’s performance. For instance, the measurement method to report absolute
efficiency for high-purity Ge (HPGe) detectors (see Chapter 20) is outlined under ANSI/IEEE 325-1996,
which describes a standardized distance, orientation and radiation energy. However, for general use, the
characterization of a detector by its absolute efficiency may be difficult to repeat.
Relative efficiency R is the absolute efficiency of a test detector compared directly with another reference
detector of known absolute efficiency refA under identical conditions, i.e.,

A Rdet
R = = n . (7.2)
ref
A ABref
A i=1 Ci

Typically, the reference detector is an established standard. For instance, using the HPGe example once
again, the ANSI/IEEE 325-1996 standard prescribes that the HPGe detector be compared directly to the
performance of a 3-in. × 3-in. right-cylindrical NaI:Tl detector (see Chapter 13), where the established
absolute efficiency for the NaI:Tl detector is 1.2 × 10−3 [Fairstein et al. 1996]. Commercial vendors com-
monly quote relative efficiencies for various detectors; hence, it is important that the user understand the
characterization method used to determine the efficiency.
Intrinsic efficiency I is the ratio of the detector response (counts or count rate) to the particle emission
or emission rate further divided by the solid angle Ω subtended by the detector with respect to the (point)
source divided by the 4π solid angle of radiation emission, i.e.,

4πA 4πRdet
I = = n . (7.3)
Ω ABΩ i=1 Ci

Here Ω is proportional to the probability that emitted radiation intersect the detector’s entrance aperture.
For the case that the radiation source is not a point source, Ω/4π is replaced by a correction factor PF which
is again the probability the emitted radiation is in a direction toward the detector aperture. The intrinsic
efficiency is often reported in an attempt to reduce the dependence upon system geometry, by considering
only the radiation that is emitted toward the detector. Intrinsic efficiency, can, in principle, be used to scale
the expected absolute efficiency for various alternate source/detector geometries.
Although the use of intrinsic efficiency mitigates the geometric dependence on efficiency measurements,
it does not completely eliminate this dependence. Other effects such as the source preparation, detector
characteristics, and the medium between the source and detector can also affect the measured results. These
various effects that alter the measured efficiency can be classified into the following three broad categories.

Source Effects: The source preparation and encapsulation can alter the energy and number of radiation
particles arriving at the detector aperture.

Detector Effects: The operational characteristics of a detector can alter the measured energy and number
of radiation particles recorded by the detector.

Geometric Effects: The geometry of the source, detector and their configuration with respect to each
other affect the energy and number of radiation particles arriving at the detector aperture.

These topics and how to correct for them are discussed in the remainder of this chapter.
Sec. 7.2. Source Effects 245

7.2 Source Effects


Preparation of the source material and its encapsulation has an effect on the emission rate of radiation from
the source assembly. Both alpha and beta particles sources can suffer significant backscatter from the source
backing, or can also have considerable energy attenuation if the source material or source encapsulation is
too thick. Likewise, the material (such as air) between the source and detector and the detector window
reduce the number and energy of particles reaching the sensitive volume of the detector. Measurement
of gamma rays and neutrons may produce significant room scatter if the shielding around the detector is
inadequate. However, even with shielding to prevent room scatter, scattering from the shielding material
itself produces scattered particles than can still reach the detector. Correction for all of these effects in
order to determine accurately the source strength from a measured detector response is a formidable task.
However, with proper source and detector designs, the needed correction factors can be made small (a few
percent) so that approximate estimates of them can suffice.
detector
Consider an idealized source/detector geom- backing
etry shown in Fig. 7.1 in which the source mate- source

rial, the source substrate or backing, the source d protective


encapsulation cover and the detector window cover

consist of parallel planes. As shown, there are


many possibilities for source radiation to be pre-
vented from reaching the active volume of the
detector and also possibilities for which emitted
radiation that would miss the detector can be
redirected into the detector. To address all of
the possibilities would require a detailed radia-
tion transport calculation. In this section the
two most important source effects are consid- detector
ered, namely (1) self-absorption of the radiation window
by the source and (2) the backscattering of ra-
Figure 7.1. Observed counts and count rates can be affected
diation from the source substrate. These effects by source and detector effects, including backscattering off of the
are addressed using simple and, thus, approxi- detector window, backscattering off of the source backing, and at-
mate analyses and are based on several key as- tenuation through the source material, source window, medium
between the detector and source, or detector window.
sumptions such as straight-line radiation trajec-
tories, exponential or finite range attenuation, no source cover, a radionuclide source with isotropic emission,
and a detector response that is insensitive to the energy and angle of incidence of the entering radiation.
First a few key parameters are defined and then results for different types of radiation are given.
Source Self-Absorption Effect
Define the self-absorption factor for a source layer of thickness d
no. particles exiting the source
fa (d) ≡ , (7.4)
no. particles exiting without self-absorption
where only particles emitted towards the front surface (i.e., the surface adjacent to the detector are consid-
ered). This factor is the probability Paesc (d) that a particle born uniformly in the source volume escapes
through the front surface. Division of the measured source strength Smeas , inferred from the detector count
rate, by fa gives a source strength corrected for source self-absorption that is larger than Smeas because fa
is always less than unity.
As d → 0 the self-absorption factor fa (d) → 1, i.e., there is no self-absorption and all source particles
escape the source layer. It should be noted that both the energy and angular distributions of the escaping
246 Source and Detector Effects Chap. 7

particles are, generally, different than those particles emitted by the radionuclide. Also the self-absorption
factor cannot be measured experimentally since all sources must be composed of matter and, thus, be capable
of interacting with the radiation.
Source Backscatter Effect
Radiation particles emitted by the source in directions away from the detector can reach the source backing,
of thickness T , in which they can scatter and some are subsequently reflected back towards the detector. To
correct Smeas for this backscatter effect, a backscatter factor fb (T ) is defined as
no. particles recorded with source backing
fb (T ) ≡ . (7.5)
no. particles recorded without source backing
To evaluate fb (T ) it is assumed there is negligible source self-absorption so that half of the source particles
S leave towards the detector and half impinge on the source backing. Because the recorded count rate is
proportional to the rate at which particles leave the source in the direction of the detector, the backscatter
factor is given by
0.5S + 0.5S ηb (T )
fb (T ) = = 1 + ηb (T ), (7.6)
0.5S
where ηb is the reflection coefficient and is the probability a particle entering the substrate is reflected back
to the surface.
This coefficient increases from 0 to a saturation value ηb as the thickness of the source backing increases
from 0 (no backscattering) to a value beyond which negligible particles are reflected. For particles with a
finite range Ref f saturation reflection is achieved when T = Ref f /2 since no particles can reach a greater
depth and return to the backing surface. In practice, T  0.3Ref f achieves saturation reflection. For particles
that are exponentially attenuated with an attenuation coefficient μ, T  1/μ results in near saturation. The
reflection coefficient usually is a measured quantity, although with modern Monte Carlo transport techniques
it can be calculated.

7.2.1 Alpha Particles


The preparation of the radioisotope that emits alpha particles can affect the observed count rate and spec-
troscopic energy resolution. If the radioisotope is deposited as a thick layer, the alpha particles lose energy
as they travel through the source material. The energy loss depends on the alpha-particle trajectory and
where in the source material the particle was emitted. Likewise particles emitted towards the material upon
which the radioisotope was deposited can make multiple Coulombic scatters and be reflected back towards
the detector. This backscatter component can cause an overestimation of the source activity by increasing
the count rate over that expected from a source with no backing.
In some cases, alpha-particle sources have a protective covering to reduce risk of contamination from
radioisotope leakage. These thin windows, as well as the detector window, can cause alpha particles to scatter
away from the detector, thereby causing an underestimation in the source activity. Further, thin windows
can absorb energy from the particles, thereby reducing the range and measured energy while increasing the
uncertainty for spectroscopy measurements. To minimize the effect of the detector window a thin form of
boPET1 is typically used for alpha-particle source windows and detector windows, thereby, reducing both the
effects of energy loss and backscattering. These multiple measurement problems are illustrated in Fig. 7.1.
Finally, if there is a medium, such as air, between the source and the detector window further degradation
of the energy of the alpha particles occurs.

1 Biaxially
oriented polyethylene terephthalate (boPET) is a stretched polyester film commonly known by trade names such as
Mylar. Applied as detector windows, these films are generally between 3 to 6 microns thick (or 0.4 to 0.8 mg cm−2 ), and
being primarily composed hydrogen, carbon and oxygen (C10 H8 O4 ), alpha-particle backscattering is minimal.
Sec. 7.2. Source Effects 247

Attenuation
Consider the arrangement, shown in Fig. 7.2, in which an alpha particle source of thickness d, plated upon
a planar backing, is placed inside the chamber of a gas-filled detector, such that half of the emissions are
initially emitted towards the gas, the other half being emitted in the direction of the backing. Under ideal
conditions, half of the emissions should be detected.2 However, particles emerging at oblique angles from
the normal (perpendicular) trajectory may pass through so much material that they lose too much energy
for detection.
Recall that alpha particles have discrete ranges in Detector Medium
matter, denoted here as Ro  RCSDA , about which
there is a minimal amount of straggle. As alpha parti-
cles are emitted in the source material, they lose energy
before emerging into the detector. At some critical an- q
gle θ the alpha particle has just enough energy to still d Reff R0 Rz x
be detected as it emerges from the source material, a Plated Source
condition that is dependent on the alpha-particle tra-
jectory and the detector electronic lower level discrim-
inator (LLD) threshold (Eα ≥ ELLD ). This effective Source Backing
range Reff is the maximum distance that the alpha
particle can travel through the source material before
Eα < ELLD , i.e., Figure 7.2. Depicted are the average total range Ro and
the average effective range Reff of alpha-particle emissions
Reff = Ro − Rz , (7.7) from a plated source of thickness d born at location x.

where Rz is the residual range, the range in the source material that an alpha particle with energy ELLD
would have.
Consider an alpha particle emitted at depth x in the source material. Because the emission is isotropic,
the probability it reaches the source surface with sufficient energy to be detected is pesc (x) = ΔΩ(x)/4π,
where ΔΩ(x) is the solid angle subtended by the disk on the surface defined by the cone with the half-angle
θ in Fig. 7.2. A differential solid angle in spherical coordinates (see Section 7.4) is dΩ = sin θ dθ dψ where θ
is the polar angle and ψ is the azimuthal angle. Hence
  2π  θ  
x
ΔΩ(x) = dΩ = dψ sin θ dθ = 2π(1 − cos θ) = 2π 1 − . (7.8)
0 0 Reff
Note that if x ≥ Reff , pesc (x) = 0 because either no particles can escape the source material or escaping
particles have energies below ELLD and cannot be detected. Then the probability Pa an alpha particle born
uniformly within the source material escapes attenuation from the source material is given by
 min(d,Reff )
esc
Pa = {probability an alpha particle is emitted in dx about x}×{pesc(x)}. (7.9)
0

Because the radioisotope is distributed uniformly in the source material, the probability an alpha particle is
emitted in dx about x is dx/d so that
 min(d,Reff ) " # " #  min(d,Reff )  
dx ΔΩ(x) 1 x
esc
Pa = = 1− dx. (7.10)
0 d 4π 2d 0 Reff

2 Sucha detector is often referred to as a 2π detector, because the source emits particles into the detector chamber over a solid
angle of 2π steradians.
248 Source and Detector Effects Chap. 7

Evaluation of the integral yields




⎪ 1
1−
d
⎨ , if d < Reff
2 2Reff
Paesc = . (7.11)


⎩ Reff , d ≥ Reff
4d
In the above analysis it was assumed that the source material composition is known so that the ranges
Ro and Reff are known. Unfortunately, the chemical form of the source material is seldom known because
source manufacturers often regard this information as proprietary.
Attenuation of alpha particles through the intermediate medium between the detector and source, typ-
ically air, causes energy loss and range reduction. Alpha particle detectors must be placed close enough to
the source such that the particles can enter the detector medium with sufficient energy to be detected. In
the prior case of the 2π detector, the alpha-particle source is placed inside the detector cavity. However,
operation of common survey meters and thin-window detectors does not permit such a placement, and the
sensitive detector volume must be placed within the range of the alpha particles. Further, the thin window
of the device must be taken into account as part of the total range reduction.
The total energy attenuation becomes a function of the source thickness, the medium distance between
the detector and source, and the detector entrance window thickness. Often it is the “mass thickness” of a
material that is quoted for range (see Fig. 7.3), defined as the product of the alpha-particle range and the
mass density of the attenuating material, i.e., Rmass = ρRo g cm−2 .
Backscattering
Consider the backscatter events shown in Fig. 7.1. From the general expression for Rutherford
backscattering [Kaplan 1962], it is unlikely that an alpha particle backscatters towards the detector
from a nucleus in the source backing material in a single scattering event. Instead, it is multiple
small-angle scatters that can cause the alpha par-
ticle, originally on a trajectory towards the source
backing, to eventually emerge from the source
towards the detector. The overall consequence
of alpha-particle backscattering is to produce a
10 -2
higher count rate than that without backscat-
Mass Thickness (g cm )

tering. Hence a backscattering correction factor


-2

Lead should be estimated and used when reporting the


measured source activity.
Silver Careful source preparation may allow an ex-
Silicon
perimenter to produce an ultra-thin source back-
Germanium
10 -3
ing, which produces minimal backscattering, and,
thereby, effectively eliminates the backscattering
Carbon
problem. However, repeatability of source prepa-
Helium ration often becomes an issue, compounded by
calibration issues. Instead, it is far more com-
mon to prepare sources that reach a saturation
10 -4 backscatter limit. Intuitively, to achieve this
0.1 1 10
limit, the source support (backing) should be
Alpha Particle Energy (MeV)
≥ Ro /2 for the backing material; hence, a par-
Figure 7.3. Alpha particle mean range Rp as a function of ticle scattering deeper than Ro /2 cannot emerge
mass thickness and energy (from Ziegler, 2013).
from the backing material.
Sec. 7.2. Source Effects 249

A general expression for alpha-particle backscattering is [Crawford 1949]


 %N 1/2
2
i=1 fi Ai
3/2 %N
ηb = K 1/2
, (7.12)
Ar i=1 fi Ai

where ηb is the probability that a particle is backscattered if it is emitted in the direction of the source
backing, K is a constant, Ar is the atomic weight of a reference backing material, Ai are the atomic weights
of the constituents in the backing material (or window material), and fi are the atomic fractions of the
elements (see also [Deruytter 1962]). For elemental source backings, Eq. (7.12) reduces to
3/4
A
ηb = K . (7.13)
Ar
From Eq. (7.13), the amount of backscatter increases as A (or Z) increases, indicating that low Z materials
are best used for alpha-particle source backing.
Reported experimental results indicate that the alpha-particle backscatter probability measured with
210
Po (Eα = 5.307 MeV) is [Hutchinson et al. 1968]
(1.30 ± 0.08) × 10−3 Z
ηb = , (7.14)
C0
where C0 is a constant measured to be 2.525 ± 0.002. Variations with alpha-particle energy and the thickness
of the backing material were not considered in Hutchinson’s work; presumably, saturation backscatter coef-
ficients were investigated and measured. According to Eq. (7.14), a 5.31-MeV alpha-particle source on an
Al backing has a 0.67% backscatter coefficient, while the same alpha-particle source applied to a Au backing
has a 4.07% backscatter coefficient. Hutchinson et al. [1968] also report that the surface morphology of the
source backing affects the backscatter coefficient, ηb being generally higher for polished source backings as
opposed to unpolished source backings.
With the source of sufficient thickness to reach the asymptotic backscatter limit, Rossi and Staub [1949]
approximate the backscatter probability as

ηb  0.201φ, (7.15)

where φ is a function of the effective range in the backing material, defined as Re = Ro − Rz . To some
degree, Eq. (7.15) takes into account the energy of the alpha particle, in which ηb is dependent upon the
necessary effective range Re . Rossi and Staub [1949] published a short table of values for φ that can be used
to estimate ηb .
Little, if any, experimental data is available about the energy distribution of the alpha particles that are
backscattered from the source backing. However, with modern Monte Carlo methods it is now possible to
track alpha particles as they undergo Coulombic scattering and estimate ηb and the energies of backscattered
alpha particles from any backing material. Example calculations are shown in Fig. 7.4 for an isotropic
source. Notice the energy spectra are peaked towards very lower energies (for alpha particles that penetrated
relatively far into the backing and took many small-angle scatters to re-emerge) and at energies close to the
source energy (from particles that entered the backing at grazing angles and, hence, needed only a few
scatters to re-emerge). The area under each histogram gives ηb . For example, for aluminum ηb = 0.83%.
However, if the low-energy reflected alpha particles below 0.5 MeV are ignored, then ηb = 0.67%, a result in
agreement with Hutchinson’s measured value quotes from above.
MCNP6 has been used to calculate the total backscattering probability for different backing materials
(see Fig. 7.5). The variation of ηb (sat) with the Z number of the backing medium is well described, as shown
250 Source and Detector Effects Chap. 7

Figure 7.5. The saturation backscatter probability for alpha


particles as estimated with MCNP6 [2013] (solid circles) as
a function of the backscattering material Z number. The
Figure 7.4. A histogram of the number of 210 Po alpha associated uncertainty is less than 0.5% for all points. Here E
particles backscattered from three thick metal surfaces. En- is the initial energy of the alpha particle and the energies 3.18
ergy bin widths are 0.01 MeV. Results obtained with MCNP6 MeV, 5.30 MeV, and 8.78 MeV are the energies of the alpha
[2013]. particles emitted by 148 Gd, 210 Po, and 212 Po, respectively.

by the solid lines in Fig. 7.5, by the simple relation ηb (Z) = aZ b , where a and b depend on the initial energy
Eα of the alpha particle. Based on MCNP6 calculations shown in Fig. 7.5, the probability of backscattering
is approximately (see the dashed lines in Fig. 7.5)

ηb (Eα , Z)  Z 0.595 exp(−5.63 − 0.132Eα ), (7.16)

where Eα is the initial energy of the alpha particle (in MeV).


In general, when performing alpha-particle measurements, the experimenter should correct the acquired
count rate g, and hence the measured activity, by using a backscattered corrected count rate g̃
g g
g̃ = = . (7.17)
1 + ηb fb

7.2.2 Beta Particles


As with alpha-particle sources, beta-particle sources can also suffer from attenuation (self-absorption) in the
source material and its encapsulation and from backscatter effects. This latter effect can be particularly severe
for backscattering from heavy elements. Hence, correction for these effects is important to measurement
accuracy.
Attenuation
Consider a volume of source material of thickness d in which beta-emitting radionuclide is uniformly dis-
tributed. At any depth x in the source material beta particles are emitted isotropically with a continuum
of energies up a maximum energy Emax such that χβ (E) dE is the probability the beta particle (either an
Sec. 7.2. Source Effects 251

electron or positron) is emitted with energy in dE about E. The probability a beta particle reaches the
surface of the source material and is not absorbed in the source film can formally be written as
 Emax  π  d
Paesc = χβ (E)dE dθ dxfβ (x, θ, E), (7.18)
0 0 0

where fβ (x, θ, E) is the probability a beta particle emitted at depth x with energy E reaches the surface
traveling in direction θ with respect to the surface normal. However, there is no analytical solution or
even numerical solution of Eq. (7.18), because there is no known expression for fβ (x, θ, E). Unlike the
case of alpha particles which travel in straight lines with a well-defined range, beta particles travel along
twisted trajectories (see Fig. 4.22) that can terminate at any distance from the emission point up the
continuous slowing down approximation (CSDA) range of the beta particle. To evaluate Paesc accurately for
beta particles, it is necessary to employ Monte Carlo methods.
Although not strictly accurate, the attenuation of beta par-
ticles through a material can sometimes be modeled by an ex-
Plated ponential function
Source I(x)
= I0 e−μx , (7.19)
I0
L where I(x)/I0 is the fraction of the initial ionization measured
Source (say) by an ion chamber after the beta particles have passed
Backing
qc through an absorber of thickness x and μ is an effective linear
attenuation coefficient. Note that Eq. (7.19) is not based on
a physical phenomenon, but instead is derived from rather re-
markable linear fits of beta-particle transmission data plotted
upon semilogarithmic graphs [Baltakmens 1970].3 An empir-
ical relation that gives the mass absorption coefficient ρμ is
[Evans 1955]
μ 17
= 1.14 cm2 g−1 , (7.20)
ρ Emax
d x 0 where Emax is in MeV. This mass absorption coefficient only
Figure 7.6. Geometry for a beta-particle source.
weakly depends on the Z number of the absorber increasing
slightly with Z.
Consider the beta source shown in Fig. 7.6 with thickness d in which beta particles can be emitted from
any depth x in the film. Assume that Eq. (7.19) is an adequate estimate for beta-particle attenuation,
thereby removing the energy dependence in Eq. (7.18). Further, assume that the beta particles travel an
average distance L from their emission point (an average over the beta energy spectrum). Then the escape
probability for a beta particle emitted at depth x is the fraction emitted into a cone of directions with
half angle θc = cos−1 (x/L), namely ΔΩ(x)/4π (see Eq. (7.8)) times the probability the beta particle is not
exponentially attenuated on the way to the surface, i.e.,
     
1 θc (x) min(L,d) x x
Paesc = 1− exp −μ d − dx dθ. (7.21)
2 0 0 L cos θ(x)

Even numerical evaluation of this result is difficult because average ranges L for a beta spectrum are gen-
erally unknown. But more important, this approach based on exponential attenuation of beta particles

3 Exponential attenuation implies an infinite range which is not true for beta particles. Equation (7.19) applies only to the
initial portion of the attenuation curve.
252 Source and Detector Effects Chap. 7

along a straight line to the source surface is approximately true only for the initial portion of the intensity
versus penetration relation. Moreover, this approach does not address the change of the energy spectrum
and angular distribution of the escaping electrons. However, many texts (including this one) continue to
propagate this questionable approach, primarily because of its simplicity and the avoidance of a full-blown
electron transport calculation.
Backscattering
An empirical formula for the backscatter coefficient for normally-incident monoenergetic electrons was pro-
posed by Tabata et al. [1971], namely

b1 exp[−b2 Z −b3 ]
ηb = , (7.22)
1 + (b4 + b5 Z −b6 )τ b7 −(b8 /Z)

Table 7.1. Constants for the determination of beta- where τ = Eβ /(me c2 ). Here Eβ is the initial energy of the
particle backscattering. From [Tabata et al. 1971]. beta particle, Z is the atomic number of the target mate-
Constant Value Constant Value rial, me c2 is the rest mass energy equivalent of an electron,
and the constants a1 through a8 are listed in Table 7.1.
b1 1.15 ± 0.06 b5 15.7 ± 3.1
b2 8.35 ± 0.25 b6 1.59 ± 0.07
For energies from approximately 50 keV up to 22 MeV,
b3 0.525 ± 0.020 b7 1.56 ± 0.02
and for Z ≥ 6, Eq. (7.22) has  7% RMS deviation from
b4 0.0185 ± 0.0019 b8 4.42 ± 0.18 the data measured by Tabata et al. [1971]. The results of
Eq. (7.22) for several elements are shown in Fig. 7.7. Al-
though Eq. (7.22) is often used for backscattering of beta particles emitted isotropically from radioisotopes,
it is based on experimental data in which electrons were normally incident on the substrate. As calculated
by Kuzminikh and Vorobiev [1975] the backscatter coefficient varies strongly with the incident angle with
respect to the surface normal and ηb increases as the incidence angle increases. Because beta particles are
emitted isotropically, an uncollimated source will produce a different average backscatter coefficient than
described by Eq. (7.22). Thus, Eq. (7.22) likely underestimates ηb , but its use for beta particles, which are
incident at all angles, is continued for lack of an alternative.




 










 

 

     
   

Figure 7.7. Calculated beta-particle backscatter coefficients as functions of target Z and beta-particle
energy (after Tabata [1971]).

Monte Carlo Correction Factors


For beta particles, the only accurate way to account for source back scattering and attenuation by the
source encapsulation is to use electron transport techniques. Several Monte Carlo codes are available to
perform such calculations. Many use condensed-history models, but some are now able to use point-wise
Sec. 7.2. Source Effects 253

Figure 7.8. The MCNP6 calculated energy spectrum of electrons


leaving a 1.55 × 2.54 mm plastic disk containing a 90 Sr/90 Y beta
particle source in the center of the disk. In this example, 0.638
electrons are emitted by the disk per source beta particle.

electron interaction models. Another advantage to this approach is that both the backscatter and source
encapsulation effects can be determined in a single calculation. Moreover, the energy spectrum of the emitted
beta particles and electrons can be found at the same time. In Fig. 7.8 the emitted spectrum from a common
90
Sr/90 Y check source is shown.

7.2.3 Penetrating Radiations (γ rays, x rays, neutrons)


Although penetrating radiations, such as gamma rays, x rays, and neutrons, can all have backscatter and
attenuation effects from the source, these effects are generally small and ignored. The exception may be
for low-energy photons in heavy encapsulation. However, scattering from walls, floors and other massive
objects in the room can make a significant difference in a radiation measurement, especially when dealing
with neutron sources.
Often shielding is placed around and in close proximity to the source and detector to reduce roomshine
and background from radiation sources outside the counting chamber. This shielding is important if a
correct measurement of the source activity is to be obtained. Standard lead bricks are often used to provide
such shielding. However, for photon sources, such shielding can emit copious 88-keV fluorescence when
source photons photoelectrically interact with the lead. To minimize this secondary radiation, the counting
chamber can be lined with metals of decreasing Z values, e.g., copper followed by aluminum. To design
proper shielding and to correct for roomshine, transport codes must generally be used.

7.2.4 Source Decay During Measurement


A measurement taken in the presence of a radiation background overestimates the result for any sample
under investigation. As covered in Chapter 6, corrections for the background counts or background count
rate, and the associated error, must be considered for any radiation measurement.
254 Source and Detector Effects Chap. 7

If background is negligible by comparison to the radioactive source emission rate, but the radioactive
source under test suffers appreciable decay during the measurement time t1 , i.e., λt1 > ∼ 0.01, then the count
rate n0 at starting time t0 can be determined from the total observed counts recorded between t0 and t1 .
Consider the simple case of a radionuclide sample of N0 identical radionuclides at time t0 . The decay constant
is λ and the radionuclides emit a single particle per decay, i.e., the frequency or branching ratio per decay is
1. Further, the detector efficiency for recording this particle is denoted by . The count rate n(t) at t ≥ t0 is

n(t) = λN0 e−λt (7.23)

The average count rate n between t0 = 0 and t1 is



λN0  t1 −λt n0 −λt1
n= e dt = − (e − 1), (7.24)
t1 0 λt 1

where n0 = λN0  is the count rate at t0 . Rearrangement gives

λt1
n0 (t0 ) = n . (7.25)
1 − e−λt1
Finally the count rate at any time t > 0 is
λt1
n(t) = n e−λt . (7.26)
1 − e−λt1
This result applies to the more usual case in which the radionuclide emits M particles, each with a
different energy. Denoting the emission frequency of the ith particle by fi and the detector efficiency for the
ith particle by i yields the initial count rate n0 as


M
n0 = λN0 i fi . (7.27)
i=1

7.2.5 Contamination
As a final word on errors associated with radioactive samples and preparation, there is always the possibility
of contaminating the detector work area and/or detector with radioactive material. Radioactive sources that
produce airborne daughter products (222 Rn for instance) can contaminate the detector aperture, a situation
that causes the detector itself to become a background radiation source. Alpha particle sources are sometimes
encapsulated with a boPET thin film to reduce leaks and contamination, which unfortunately reduces their
use as spectroscopy standards. Gamma-ray and many beta-particle sources can be encapsulated in plastic
to reduce the risk of contamination. As a precaution, radioactive sources should be checked periodically for
leaks.

7.3 Detector Effects


7.3.1 Scattering and Absorption by the Detector Window
For almost all radiation detection systems the source is located outside the sensitive volume of the detector
which is enclosed in some housing. Radiation then must enter the detector through a window or aperture.4

4 There
are exceptions. For example, gas flow proportional counters and some liquid scintillators have the source in the detecting
medium.
Sec. 7.3. Detector Effects 255

As radiation particles reach the detector window, most pass through into the sensitive detector volume and
are recorded. But a small fraction are either absorbed or scattered back by the window material as depicted
in Fig. 7.1. Even if a particle passes through the window it may lose sufficient energy in doing so that
the signal produced by it falls below the lower level discriminator (LLD) setting and so the particle is not
recorded.
Correction for window effects is very difficult because such corrections depend on the type of radiation,
its energy, its angle of incidence to the window, the window material, and the window thickness. Because of
this complex dependence, there is no direct way to correct for window effects. However, to minimize window
effects one should make the window as thin as possible and of a material that is as transparent as possible
to the incident radiation. For low-energy photons and changed particles windows of low Z material are
generally better than those made from high Z materials. For neutron detectors, window materials with very
small neutron cross sections at the neutron energies of interest are preferred. Common window materials
are boPET, glass, mica, or low-Z metals. Often the absorption effect of the window is incorporated into the
efficiency of a detector. But for an energy spectrometer, corrections for energy loss in the window must be
made separately to the spectrum.

7.3.2 Time Interval Distribution between Radioactive Decays


The times at which interactions occur in a detector from particles emitted from a radioactive (or stochastic)
source have a Poisson distribution (see Section 6.7). The mean or expected rate at which interactions (or
events) occur is denoted by r̄. In a time interval t the mean number of events is, thus, μ = r̄t with a variance
of μ. Thus, the probability of having n events in time t is given by
(r̄t)n −r̄t
P(n|μ) = e . (7.28)
n!
In the following section on dead time, information about the time intervals between events is needed. In
particular, the probability there is no event in a time t following an event, P0 (t). From the Poisson PDF,
the probability that no events are observed within a time interval t is
0
(r̄t) −r̄t
P(0|r̄t) = e = e−r̄t . (7.29)
0!
The probability that an event occurs within some differential time interval dt about t is expressed as r̄dt.
From these two results, it follows that the probability of observing no event in the time interval (0, t) and
an event in the next dt interval is
: ;
dP0 (t) = e−r̄t (r̄dt) = r̄e−r̄t dt. (7.30)

Therefore, the total probability that there is no event within time t is expressed as the probability that the
event occurs anytime time past t, i.e.,
 ∞  ∞
P0 (t) = dP (t) = r̄e−r̄t dt = e−r̄t . (7.31)
t t

The probability that there are one or more events within time t is then [1 − exp(−r̄t)].

7.3.3 Dead Time


All radiation detection systems operating in pulse mode have a limit on the maximum rate at which data
can be recorded. The limiting component may be either the time response of the radiation detector, which
is usually the case for the Geiger-Müller counter, or may be the resolving capability of the electronics.
256 Source and Detector Effects Chap. 7

1 2 3 4 5 6 7
Linear 7 interactions
Model recorded

t
Non-Extendable 5 interactions
Model recorded

t
Extendable 4 interactions
Model recorded

Time

Figure 7.9. The three basic models for detector interval operation. The linear model assumes
that the pulse is a delta function and has no processing time and, hence, has no dead time. The
non-extendable dead time model assumes that once a pulse is registered, a preset time interval τ
must pass, before another event can be processed. The extendable dead-time model assumes that
each pulse entering the system restarts the dead-time interval, even during a previously initiated
dead-time interval (after NCRP, 1985).

Although a radiation counting system is treated as a system that counts radiation interactions in a
detector, it is instead actually recording the number of detector response time intervals initiated by a
radiation particle, each time interval being terminated by the interval processing time. In other words, the
detector records intervals rather than events. If two radiation particles interact within the detector during
a single processing interval, only one of the interactions is recorded.
After a radiation interaction, radiation detectors generally require time to reset before they are fully
sensitive to record a subsequent radiation interaction, especially for pulse mode operated electronic detectors.
The time during which a detector is insensitive is commonly referred to as dead time, although the term is
often misused. Dead time actually refers to a time duration in which a detector in insensitive to a radiation
interaction. Resolving time is the period required before the detector can form a signal pulse large enough to
register in the detector system, and is dependent upon the detector characteristics and the preset electronic
conditions (lower level discriminator setting, pulse shaping time, etc.). The recovery time is the period
required after a radiation interaction for the detector to reset to its initial starting condition. Often the dead
time and resolving time are interchanged. Although technically different, the overall effect of either dead or
resolving times on the radiation counting system is the same. Detector insensitivity and dead-time issues
can arise from many sources, such as limitations in pulse processing times, limitations in detector signal
formation, and time constants required for the device to return to its full sensitivity. The details of pulse
processing are saved for Ch. 22 on nuclear electronics. In the present section, the effect that dead time and
resolving time have on a radiation measurement is presented. Also, because both dead time and resolving
time have the same effect on a radiation measurement, for simplicity, both are referred to in this chapter as
dead time.
When a radiation interaction occurs in a detector and produces a measurable event, the detector and
counting system become occupied while processing the event. As a consequence, the counting system does
not respond to a subsequent event until some time τ has passed. Because the counting system is unavailable
for a portion of time during a measurement, the recorded number of counts is consequently less than the
number of interactions that actually occurred in the detector during the measurement time. Three possible
ways in which a counting system processes a radiation event are shown in Fig. 7.9.
Sec. 7.3. Detector Effects 257

Figure 7.10. The three basic models for detector interval operation. The
linear model assumes no processing time, hence has no dead-time losses. The
non-extendable dead-time model shows a gradual reduction in the observed
events gτ as the interaction rate nτ increases. The extendable dead-time re-
sponse has a maxima in observed events as the interaction rate nτ increases,
beyond which the observed event rate gτ decreases. Note that the extendable
model produces for a single observable event rate, g1 τ , two possible interaction
rates (shown as n1 τ and n2 τ ).

7.3.4 Models for Dead Time


There are three basic models regarding pulse intervals produced in a radiation detector. These models,
each with different processing times, are depicted in Fig. 7.10. The simplest is the linear model, in which
events (pulses) are treated as delta functions and there is no processing time interval associated with a
radiation event. The second model, referred to as the non-extendable (or non-paralyzing) model (NCRP,
1985; Evans, 1955), treats the intervals as preset time periods, unalterable in length by additional events
arriving during the pulse processing interval. Hence, after the time interval τ begins, it remains the same
length regardless if more events interact in the detector during the interval τ . The third model, referred to
as the extendable (or paralyzing) model, treats an initial pulse interval τ as being restarted with another
time τ for subsequent interactions arriving during the entire pulse interval. Hence, regardless of when in the
initial interval a previous radiation interaction occurs, the interval is extended from that time forward by
τ . The total processing interval time, whether using the extendable or non-extendable model, is generally
referred to as the system dead time and denoted by τ .
Typically, the dead-time responses of detector systems consist of a combination of extendable and non-
extendable characteristics. However, most detection systems are designed in such a way that the extendable
dead-time effect is the least contributor, with the goal of producing a system that performs with non-
extendable characteristics.
Extendable (Paralyzable) Dead Time
In an extendable system, only events with time intervals greater than the dead time τ can be registered,
because there are no recorded events with time intervals less than the dead time. Suppose n represents the
true average number of events per unit time. For large n, the number of events g, per unit time, observed
258 Source and Detector Effects Chap. 7

Figure 7.11. Comparison of extendable dead time and approximations from Eq. (7.35) and
Eq. (7.37).

with intervals longer than τ is found with Eq. (7.31) to be

g = ne−nτ or gτ = nτ e−nτ . (7.32)

If the true event rate n is small, then few events are missed, and n >
∼ g. To find the exact true event rate
after observing g, n must be expressed as a function of g. Unfortunately, a closed form solution to Eq. (7.32)
cannot be found analytically. For small dead-time losses, g  n, and Eq. (7.32) can be approximated as
[NCRP 1985]
gτ = nτ e−nτ  nτ e−gτ , (7.33)

which yields
nτ  gτ egτ . (7.34)

This result can be expanded for gτ  1 as


 
(gτ )2
nτ  gτ 1 + gτ + , (7.35)
2!

which, unfortunately, underestimates nτ . However, for  = gτ  1, the following approximation compen-


sates, partially, for the underestimate
 
(gτ )2 1
1 + gτ +  (1 + )  . (7.36)
2! (1 − )
Sec. 7.3. Detector Effects 259

Substitution of this result into Eq. (7.35) gives another approximation for nτ , namely

nτ  . (7.37)
1 − gτ − (gτ )2 /2

Equation (7.37) produces a result with less than 0.1 percent error for dead-time losses of ≤ 10%. A compar-
ison of Eq. (7.32) with Eq. (7.35) and Eq. (7.39) is shown in Fig. 7.11.
For high dead-time losses, an exact solution for n can easily be found numerically by iteration. The
maximum observable event rate, gmax , for an extendable system can be found by differentiating Eq. (7.32)
and solving for maxima, i.e.,
dg
= e−nτ (1 − nτ ) = 0, (7.38)
dn
from which the maximum is seen to occur at nτ = 1. The maximum is thus

gmax = ne−1 = 0.368n. (7.39)

This result implies a dead-time loss exceeding 63% at the count rate maxima. The extendable dead-time
response function is shown in Fig. 7.10 where it is observed that the observed event rate decreases beyond
nτ = 1 even as n is increasing. The extendable dead-time response can be dangerous in high radiation
environments. An operator using a radiation detection device with extendable dead time can observe a low
count rate, when in fact the radiation environment is actually at highly dangerous levels.5

Non-Extendable (Non-Paralyzable) Dead Time


For a system with non-extendable dead-time intervals, a system is insensitive to radiation for time interval
τ directly after an event, but no longer than this time interval. Therefore, for an observed count rate g over
a measurement interval t, the system is dead for the fraction of time nτ and, therefore, the system is live for
the fraction of time 1 − nτ . The true count rate n is related to g by
g g
= 1 − gτ or n= . (7.40)
n 1 − gτ

At low count rates, gτ  1, and this last result can be approximated as

n  g (1 + gτ ) . (7.41)

As nτ increases, the maximum number of events that can be observed is limited to the maximum
number of intervals τ that fit within the counting time interval t. Hence, the maximum observed count
rate asymptotically approaches gmax = 1/τ . The non-extendable dead time response function is shown in
Fig. 7.10 where it is seen that the observed event rate continues to increase as nτ increases, asymptotically
approaching gmax .
Note that the term gτ is the fraction of the time that the detector is unable to respond to additional
ionization in the active volume of the detector. In the design of a counting system, it is best to minimize
these losses by trying, if possible, to ensure that gτ <
∼ 0.05. For example, for a GM counter with a typical
dead time of τ = 100 μs, the maximum count rate would be 500 counts/s.

5 Such an event occurred after the Chernobyl accident, when Geiger-Müller (GM) counters were used as survey meters. Ra-
dioactive core debris outside the reactor building, after the explosion, caused such high dead times that the GM counters
falsely showed low level radiation fields, when in reality the fields were dangerously high.
260 Source and Detector Effects Chap. 7

7.3.5 Counting Error Associated with Dead Time


The variance of the observed counts is often assumed to be that of a Poisson distribution and is frequently
approximated with a normal distribution. Then the observed count rate g over some counting interval t is
assumed to be the total number of true events for the measurement, i.e., N = r̄t. Such an approach is valid
for detector systems with negligible dead times in which gτ  nτ .
However, for systems with appreciable dead-time losses, those theoretical intervals Δt between events
for which Δt < τ are removed; hence, the interval distribution of recorded events does not strictly follow a
Poisson PDF and the variance must be corrected. Recall that a Poisson distribution has √ a variance equal
to the total number of observed counts, where σ 2 = gt and with standard deviation σ = gt. However, a
counting system actually records the number of time intervals registered during a measurement, and not the
actual number of events occurring in the detector. Because there are no intervals recorded for which Δt < τ ,
the actual standard deviation for nt is reduced by

σ(gt) = (1 − gτ ) gt. (7.42)

Furthermore, as derived by Vincent [1973], the standard deviation for the corrected number of recorded
counts nt is greater than the Poisson prediction by

σ(nt) = (1 + nτ ) nt. (7.43)

From Chapter 6, the net count rate is determined by n = g − b , where g is the observed count rate and
b is the observed background count rate. However, this result does not correct g and b for the detector dead
time. Denote by a subscript c the dead-time corrected rates, and assume a non-paralyzable detector, then
from Eq. (7.40) the corrected true event rate becomes
   
g b G 1 B 1
nc = g c − b c = − = − , (7.44)
1 − gτ 1 − bτ tG 1 − (Gτ /tG ) tB 1 − (Bτ /tB )

where G is the total number of counts observed over measurement time tG , and B is the total number of
background counts observed over measurement time tB . Use of error propagation, discussed in Section 6.9,
the variance is
 2  2     2  2
2 ∂r 2 ∂r 2 1 1 G 1 τ 2
σ (nc ) = σG + σB = + σG
∂G ∂B tG 1 − (Gτ /tG ) tG 1 − (Gτ /tG ) tG
    2  2
1 1 B 1 τ 2
+ + σB
1 − (Bτ /tB ) tB tB 1 − (Bτ /tB ) tB
 4  4
1 G 1 B
= + . (7.45)
1 − (Gτ /tG ) t2G 1 − (Bτ /tB ) t2B

Typically, the background count rate is small so that bτ  1, and Eq. (7.45) reduces to

 4
1 G B
σ 2 (nc ) = + 2 . (7.46)
1 − (Gτ /tG ) t2G tB
Sec. 7.3. Detector Effects 261

7.3.6 Methods for Measuring Dead Time


There are many methods of measuring the dead time of a detector system and some of the more popular
methods are outlined here. The measurement of dead time may be dictated by the availability of sources
and equipment. The user is advised that these methods vary in accuracy; hence, the choice of a method may
also be dictated by how much error is acceptable.

Two Source Method


The determination of dead time by the two source method is a simplification of the multi-source method. Two
nearly identical calibrated sources are used in this measurement method. Often these sources are available
as “split pairs.” For instance, the two sources in a split-pair beta-particle source, identified as sources 1 and
2, are often conveniently shaped as two halves of a disc.
Sources 1 and 2 are measured independently in the system to yield count rates 1 and 2, or g1 and
g2 . Afterwards, both sources are measured together to produce a combined count rate g12 . In order to
reduce possible geometric anomalies from source placement, a common practice is to place one source in the
detection location for measurement, followed by a second source, and finally the removal of the first source.
For instance, source 1 is located in the detection region to measure g1 . Next, the second source is carefully
placed next to the first source to measure g12 . Afterwards, the first source is carefully removed, so as to not
disrupt the location of source 2, in order to measure g2 . A background measurement then follows.

Non-Extendable Dead-Time Model First consider a detector with a non-extendable dead time. The true
event rates for each measurement are related by

nc1 − ncb + nc2 − ncb = nc12 − ncb . (7.47)

With the use of Eq. (7.40) and Eq. (7.44), this result yields

g1 g2 g12 b
+ = + . (7.48)
1 − g1 τ 1 − g2 τ 1 − g12 τ 1 − bτ

An approximate solution for the dead time τ can be found by use of the approximation, valid for gτ  1,
namely
g
 g(1 + gτ ). (7.49)
1 − gτ
Equation (7.48) then becomes

g1 (1 + g1 τ ) + g2 (1 + g2 τ )  g12 (1 + g12 τ ) + b(1 + bτ ), (7.50)

which is readily solved for τ to give

g12 + b − g1 − g2
τ . (7.51)
g12 + g22 − g12
2 − b2

However, Eq. (7.51) can introduce significant error because it is based on a first order expansion. Equa-
tion (7.48) can be rearranged to produce the following quadratic equation

(g1 g2 (g12 + b) − g12 b(g1 + g2 )) τ 2 − 2 (g1 g2 − g12 b) τ + (g1 + g2 − g12 − b) = 0, (7.52)


262 Source and Detector Effects Chap. 7

whose solution for the smaller of the two positive roots is

1   
τ= −B − B 2 − 4AC , (7.53)
2A

where A = g1 g2 (g12 + b) − g12 b(g1 + g2 ), B = 2 (g12 b − g1 g2 ), and C = g1 + g2 − g12 − b.


This expression for τ can be simplified by the assumption that the background count rate is insignificant
(b  0). The result is
 
1/2
1 g12
τ= 1− 1− (g1 + g2 − g12 ) . (7.54)
g12 g1 g2

If the background is negligible and if g1  g2 , then in Eq. (7.48) one can approximate both (1 − g1 τ ) and
(1 − g2 τ ) by [1 − (g1 + g2 )τ /2]. With these approximations Eq. (7.48) yields the result

2(g1 + g2 − g12 )
τ= . (7.55)
(g1 + g2 )g12

Example 7.1: A split-pair source is used to determine the dead time of a common Geiger-Müller tube
detector, where the following count rates are measured:

G1 = 93, 600 counts tG1 = 60 seconds G2 = 106, 800 counts tG2 = 60 seconds
G12 = 173, 400 counts tG12 = 60 seconds B = 30, 600 counts tB = 30 minutes

Determine and compare the dead times calculated with Eqs. (7.51), (7.53), (7.54), (7.55), and (7.53).

Solution:
The estimated count rates are:

G1 93600 cts G2 106, 800 cts


g1 = tG1
= = 1560 cps g2 = tG2
= = 1780 cps
60 seconds 60 seconds

G12 173, 400 cts B 30600 cts


g12 = tG12
= = 2890 cps b= tB
= = 17 cps
60 seconds (30 minutes)(60 sec/min)

Solution 1: Substitution of g1 , g2 , g12 and b into Eq. (7.51) gives

g12 + b − g1 − g2 2890 + 17 − 1560 − 1780


τ  = = 1.574 × 10−4 seconds = 157.4 μs.
g12 + g22 − g12
2
− b2 (1560)2 + (1780)2 − (2890)2 − (17)2

Solution 2: From Eq. (7.54),


   
1/2 1/2
1 g12 1 2890
τ = 1− 1− (g1 + g2 − g12 ) = 1− 1− (1560 + 1780 − 2890)
g12 g1 g2 2890 (1560)(1780)

= 9.372 × 10−5 s = 93.72 μs


Sec. 7.3. Detector Effects 263

Solution 3: The dead time is determined from Eq. (7.55) as

2(g1 + g2 − g12 ) 2(1560 + 1780 − 2890)


τ= = = 9.324 × 10−5 s = 93.24 μs
(g1 + g2 )g12 (1560 + 1780)2890

Solution 4: From Eq. (7.53), coefficients A, B and C are determined as

A = g1 g2 (g12 + b) − g12 b(g1 + g2 ) = [(1560)(1780)(2890 + 17)]


−[(2890)(17)(1560 + 1780)] = 7, 908, 063, 400
B = 2 (g12 b − g1 g2 ) = 2 [(2890)(17) − (1560)(1780)] = −5, 455, 340
C = g1 + g2 − g12 − b = 1560 + 1780 − 2890 − 17 = 433.

Substitution of these values into Eq. (7.53) gives the dead time
1   
τ = −B − B 2 − 4AC = 9.151 × 10−5 s = 91.51 μs.
2A
The exact solution, τ = 91.51 μs, was found with Eq. (7.53). The approximation calculated by Eq. (7.51),
τ = 157.4 μs, overestimates the exact answer by a factor of 1.72, a consequence of the use of a first order
expansion approximations with a relatively large value of gτ  0.15. However, the approximate value found
from Eq. (7.54), τ = 93.72 μs, overestimates the exact answer by a factor of only 1.024 (2.4%). The best
approximate value was found with Eq. (7.55), yielding 93.24 μs, noting that this approximation works only if
b g1 , g2 and g12 , and g1  g2 . It can be concluded that Eq. (7.54) can be used to calculate the dead time
provided that the background count rate is much less than the radioactive sample count rate, and Eq. (7.55)
can be used with the added stipulation that the count rates of g1 and g2 are similar. Otherwise, it is best
to use the more tedious operation required by Eq. (7.53).

Extendable Dead-Time Model The extendable dead-time model is transcendental and has no closed form
solution for τ . However, there are methods to find an acceptable approximation to the dead time, one
of which, reported elsewhere [NCRP 1985] is derived here. Assume an extendable model with negligible
background, so the true count rates are related by Eq. (7.47), namely

n1 + n2 = n12 .

The measured rates gi are then related through Eq. (7.32) as

g1 eg1 τ + g2 eg2 τ = g12 eg12 τ .

Assume that the count rates of g1 and g2 are similar, i.e., g1 τ  g2 τ so the above relation can be written as

g1 eg1 τ + g2 eg1 τ  g1 eg2 τ + g2 eg2 τ = g12 eg12 τ . (7.56)

By using only the exp[g1 /τ ] terms in this result, one can solve for τ as
g1 + g2
 e(g12 −g1 )τ ,
g12
from which  
1 g1 + g2
τ ln . (7.57)
g12 − g1 g12
264 Source and Detector Effects Chap. 7

In a similar fashion, using only the exp[g2 /τ ] in Eq. (7.56), one obtains
 
1 g1 + g2
τ ln . (7.58)
g12 − g2 g12

A better estimate of τ should be obtained by averaging these two results, namely


   
1 1 1 g1 + g2 1 (g12 + g12 − (g1 + g2 )) g1 + g2
τ + ln  2 + g g − g (g + g ) ln .
2 (g12 − g1 ) (g12 − g2 ) g12 2 (g12 1 2 12 1 2 g12

Because g1 + g2  g12 , this approximation for τ reduces to that stated by the NCRP [1985]

 
g12 g1 + g2
τ ln . (7.59)
2g1 g2 g12

This approximation for τ of Eq. (7.59) is based on the assumptions that gτ is a small number, background
is negligible, and the count rates g1 and g2 are similar. To obtain the exact solution of Eq. (7.3.6) for the
dead time, a computer program based, for example, on the bisection method can be used to iteratively arrive
at a numerical solution for τ . This numerical method can treat all values of gτ .
Pulser Methods
There may be occasions when an experimenter does not have access to a split-pair source to measure the dead
time of a detector system. For such instances, Baerg [1965] derived an approximation for non-extendable
dead-time systems which uses a periodic pulse generator (pulser) and a single radiation source. Suppose a
pulser inserts test pulses of frequency ν into the test port of the detector’s preamplifier. The pulser signal
by itself is not stochastic; however, if a radiation source is present, then the probability of observing a count
from the pulser is dependent upon the randomness of a count being registered by a radiation event, namely
(1 − gτ ). Here g is the observed source count rate without the pulser. Hence, the observed pulser count rate
p in the presence of the radiation source is p = ν(1 − gτ ).
A pulser input activates the electronics and causes the detector system to be inactive for time τ . Conse-
quently, the observed count rate g1 from the radiation source, with the pulser activated, is

g1 = g(1 − pτ ) = g(1 − ν(1 − gτ )τ ). (7.60)

The total count rate is determined by adding the probability of observing a count from the pulser with
the probability of observing a count from the radioactive source, namely

g1p = ν(1 − gτ ) + g(1 − ν(1 − gτ )τ ) = ν + g − 2νgτ − νg 2 τ 2 , (7.61)

which can be solved for τ to yield

  1/2 
1 g1p − g
τ= 1− . (7.62)
g p

Given the pulser frequency ν, the experimenter need only take measurements with (g1p ) and without
(g) the pulser to determine the dead time. Note that the assumptions used to arrive at Eq. (7.62) can lead
Sec. 7.3. Detector Effects 265

to inaccuracies in the dead-time measurements, but the accuracy is considered to be acceptable for pulser
signals with frequencies ν < 1/(3τ ) [Müller 1973, 1976].
There is no exact analytical solution for extendable dead time; however, an approximate solution for
extendable dead time with the use of a single pulser is offered by NCRP [1985], namely,

ξe−ξ
τ , where ξ = (q 2 + 4q − 1)1/2 − (q + 1) and q = ν/(g1p − g). (7.63)
g
The NCRP [1985] states Eq. (7.63) as being accurate to better than 0.3% over a wide range of pulser
frequencies, provided that gτ ≤ 0.20.
A method introduced by Baerg [1965], and described in more detail later by Müller [1973], uses two pulse
generators to measure the dead time of an electronic system without the detector. Suppose two pulsers are
used with different frequencies ν1 and ν2 , where the frequency ratio is not an integer, then an exact system
dead time is given by
gν1 + gν2 − gν1ν2
τ= , (7.64)
2gν1 gν2
where gν1 is the count rate from pulser frequency ν1 , gν2 is the count rate from pulser frequency ν2 , and gν1ν2
is the count rate with both pulsers operating. If the highest pulser frequency has ν < 1/(2τ ) then the solution
to Eq. (7.64) provides the value of τ regardless of whether the dead time is extendable or non-extendable.
However, if ν > 1/(2τ ) then Eq. (7.64) provides a method to determine if the dead time is extendable
or non-extendable. If νav is the average frequency of the combined pulsers after passing dead time τ , with
T = 1/ν ≡ min(T1 , T2 ), then the response from a non-extendable dead-time system is
$
ν1 + ν2 − 2τ ν1 ν2 , for 0 < τ < T /2 ,
νav = (7.65)
ν, for T /2 < τ < T .

For an extendable dead-time system


$
ν1 + ν2 − 2τ ν1 ν2 , for 0 < τ < T ,
νav = (7.66)
0, for τ > T .

The dead time is determined from


gν1 + gν2 − gνav
τ= . (7.67)
2gν1 gν2
A comparison of results for νav beyond τ > T /2 reveals the type of dead-time for the system [Müller 1973].
Decaying Source Method
A rapidly decaying source, such as 116m In (t1/2 = 54.2 min), is measured at incremental times as the sample
undergoes radioactive decay. The count rate is monitored, corrected for background, and plotted on a semi-
log graph. If there were no dead time, the plot would decrease linearly in time. But at high count rates
dead-time effects are important, and a plot such as that of Fig. 7.12 is obtained after the sample decays
through several half-lives.
The slope M of the linear portion of the semilogarithmic plot is then found by fitting a straight line to the
measured data. Typically, the experimenter determines this slope from a least squares fit to the lower count
rate data that yields an acceptable coefficient of determination.6 The slope M then yields the half-life from

6 Thecoefficient of determination, often denoted R2 , is an indicator of linearity for a linear regression curve fit. Values converging
on R2 = 1 are considered “perfect” predictors of an unknown variable.
266 Source and Detector Effects Chap. 7

t1/2 = ln(2)/M . This experimentally determined half-life can be compared to the literature value, thereby
providing another test for accuracy.
At the high count-rate end of the plot, the measured count rates gi underpredicts the true event rate
ni , which varies exponentially in time, because dead time prevents some events from being recorded. For a
non-extendable detector the predicted and observed count rates are related by Eq. (7.40), from which the
dead time is found to be
ni − g i
τ= . (7.68)
g i ni
Note that in the linear portion of Fig. 7.12,
ni  gi and Eq. (7.68) yields τ  0. To find
τ use the highest count-rate measurements and
the predicted true event rate
ni = n(ti ) = gn exp[λ(tn − ti )], (7.69)
where gn is an observed count rate well into the
linear portion of the decay curve. Typically, one
uses ni = n0 , the initial observation. Substitu-
tion of measured value gn and predicted value
ni into Eq. (7.68) yields τ (see Fig. 7.12).
An alternative approach is to use the decay
relation
n(t) = n0 exp(−λt), (7.70)
Figure 7.12. The dead time is determined by plotting the loga- where t0 = 0, and substitute it into Eq. (7.40)
rithm of the measured counts versus the decay time. From the plot
for a non-extendable dead-time detector to ob-
the expected values of ni are determined and the dead time τ if
found from either Eq. (7.40) or Eq. (7.32). tain [Martin 1961]
g(t) exp[λt] = −g(t) n0 τ + n0 . (7.71)
This is a linear equation, where −n0 τ is the
slope. Hence, by plotting the left-hand side of
Eq. (7.71) versus g(t) a plot similar to that of
Fig. 7.13 is obtained, from which the slope S
of the resulting straight line can be determined.
The dead time is then found as τ = −n0 /S.
For an extendable dead-time detector, the
dead time is found from Eq. (7.32), with ti = t0 ,
from the relation between n0 and g0 , namely
g0 = n0 exp(−n0 τ ). (7.72)
This result must be solved numerically. How-
ever, a similar graphical method can be used,
as described for the non-extendable dead-time
Figure 7.13. The dead time for a non-extendable detector is found case, where substitution of Eq. (7.70) into
by plotting gi exp(λt) versus gi . The slope of straight line fitted
to the data is τ n0 . Note one must wait through several half-lives Eq. (7.32) yields
until dead-time effects are negligible and an accurate value of n0 is
obtained. λt + ln(g) = −n0 τ exp[−λt] + ln[n0 ]. (7.73)
Sec. 7.4. Geometric Effects: View Factors 267

Eq. (7.73) is another linear equation in which −n0 τ is the slope. Thus, the procedure is to plot the left-hand
side of Eq. (7.73) versus e−λt , find the slope of the resulting straight line, and evaluate τ = −n0 /S.
The advantage of the graphical methods using Eq. (7.71) and Eq. (7.73) over the methods of Eq. (7.68)
and Eq. (7.72) is debatable. Both methods for finding the dead time improve as the sample is allowed to
decay through more half-lives. Regardless, these graphical estimations are generally considered inaccurate
[NCRP 1985], although accuracy can be improved by subtracting background count rates and collecting data
through enough half-lives so that dead-time effects are negligible and a reasonably accurate value of n0 can
be determined.

Increasing Power Method


The increasing power method has some similarity to the decaying source method, and requires a variable
field radiation source, such as a nuclear reactor. The detector is placed in the measurement location and
a background measurement is acquired. The radiation field is increased and measured systematically at
various power levels, preferably increasing in power if a nuclear reactor is used.7
The detector response without dead time should be linear with respect to the power level. A simple least
squares fit through the low count rate data points yields a linear function for comparison to the measured
values at high count rates. For non-extendable dead time, the difference between a linear response plotted
through the low radiation field measurements and the high field measurements yields the dead time from
Eq. (7.68), where p is the projected correct count rate from the linear fit and g is the measured count rate.
For extendable dead time, Eq. (7.72) is used. Accuracy is limited by error in the linear curve fit for low
counting rates.

7.4 Geometric Effects: View Factors


Not all radiation emitted by a radioactive source, of strength Stot particles/second, enters the detector
aperture. The fraction of emitted radiation that does enter the detector, in the absence of any radiation
attenuation between the source and detector, is called here the view factor Pv . No account of backscatter or
direction of radiation incidence on the aperture is made. The view factor is strictly a geometric probability
depending only on the shapes and sizes of the source and aperture and their relative orientation to each
other. With this quantity, the intrinsic efficiency I of the detector is

Cobs
I = , (7.74)
Stot Pv

where Cobs is the observed count rate (corrected for dead time).
Two general classes of view factors are considered in this section. The first class consists of view factors
for point isotropic sources and for plane detector apertures of simple shapes. Such sources are frequently
encountered in measurements of radioactive samples. The second class is for plane sources with different
shapes.
Finally, in this section it is assumed that source radiation is emitted isotropically, a good assumption for
most photon sources. However, the encapsulation of charged particle sources can make the emission quite
anisotropic. Such anisotropic sources are not considered here.

7 Althoughthe experiment can be conducted by starting at a high reactor power and incrementally lowering the power, it takes
much longer because a reactor’s power can be raised more quickly than it can be decreased.
268 Source and Detector Effects Chap. 7

7.4.1 Point Isotropic Sources


The view factor for an aperture of area A is closely related to the solid angle subtended at the source point
by the aperture. The basic equation for the solid angle is


n̂•dA
Ω= , (7.75)
A R2

where R is the distance between the source and dA, n̂ is a unit vector along R, n̂•dA is the area of the
projection of dA on the plane perpendicular to R. The view factor is simply Pv = Ω/4π, namely, the fraction
of the emitted radiation particles into the solid angle Ω.

Solid Angle for dA on a Sphere


Consider a radioactive point source placed at the origin
z
of spherical coordinate system, as shown in Fig. 7.14.
Given a sphere of radius r, a direction vector extend-
ing from the origin can be described by Cartesian unit dA
vectors r sin q
r r
dq
r = r sin θ cos φ i + r sin θ sin φ j + cos θ k. (7.76) q
y
Emissions isotropically radiating from the source uni- f
df
formly intersect a sphere centered about the origin. A
differentially small area dA, defined by the limits r sin θ
and r sin θ + dθ and also φ and φ + dφ through which a x
portion of this radiation passes is

dA = r sin θ dθ r dφ = r2 sin θ dθ dφ. (7.77)

Figure 7.14. Coordinate system for isotropic radia-


The solid angle is defined as dA/r2 . Integration over the tion emissions (at the origin) intersecting differential
entire sphere surface gives area dA.

   π  2π
dA
dΩ = = sin θ dθ dφ = 4π. (7.78)
4π 4π r2 0 0

This result shows that the solid angle for the entire surface of the sphere surface is 4π. The solid angle is
actually dimensionless, yet units of steradians (sr) are typically attributed to the solid angle; hence there are
4π steradians subtended by the surface of a sphere, regardless of radius r. The solid angle for a detector of
face area A can be determined with the method of Eq. (7.78).
Sec. 7.4. Geometric Effects: View Factors 269

Solid Angle for a Point Source and a Cylindrical Detector


A typical geometry for a radiation detector is a cylin-
4p Solid Angle der with radius a, as shown in Fig. 7.15. The projected
Detector Solid area (or solid angle) of the meniscus formed at the in-
Angle tersection of the cylinder and the sphere is found from
  θ  2π
1
Detector dΩ = r2 sin θdθ dφ = 2π (1 − cos θ) ,
4π r2 0 0
Source n (7.79)
q where θ is defined by the angle between a normal vector
r a n̂ and r.
Because
d
cos θ = √ , (7.80)
d2 + a2
where d is the distance from the radioactive point source
d to the center of the detector face, Eq. (7.79) becomes
 
d
Figure 7.15. Representation of the relationship be- Ω = 2π 1 − √ . (7.81)
tween a radioactive point source and a cylindrical ra- d2 + a2
diation detector of radius a with the face spaced a dis-
tance d away from the source. The fraction Pv of radiation emissions that pass through
the detector face is found by dividing the detector solid
angle by the solid angle of the sphere, namely
 
Ω 1 d
Pv = = 1− √ . (7.82)
4π 2 d2 + a2

Example 7.2:
A 3-inch × 3-inch right cylindrical NaI:Tl detector8 is placed 6 inches away from a 60 Co source for
a radiation measurement. What are the solid angle and the view factor for the detector? Assume no
intermediate absorption of the gamma rays.

Solution:
Here d = 6 inches and a = 1.5 inches
From Eq. (7.81), the solid angle is
   
d 6
Ω = 2π 1 − √ = 2π 1 − √ = 0.188 sr. (7.83)
d2 + a 2 62 + 1.52

The view factor is thus


Pv = Ω/(4π) = 0.015. (7.84)
Thus, only 1.5% of radiation emissions from the source cross the detector aperture.

8 The common notation refers to the diameter and length of a right straight cylinder.
270 Source and Detector Effects Chap. 7

Point Source Offset from Center of Circular Aperture


Consider the case of an isotropic point source set a distance d from the plane of a circular aperture of radius
a. The source is also offset by a distance s from the center of the disk. Paxton [1959] obtained analytic
solutions for the solid angle Ω subtended by the disk at the source. The view factor is thus Pv = Ω/4π. The
expressions, however, are quite complicated and involve complete elliptic integrals of the first and third kinds.
This problem is more easily obtained by Monte Carlo analyses, the results of which, for a few geometries,
are shown in Fig. 7.16.

Figure 7.16. The solid angle subtended by a circular aperture at a


point source a distance d from the aperture plane and offset from the
disk center by s. The circles are Monte Carlo results and the lines
are spline fits to data reported by Paxton [1959].

Point Source and a Rectangular Aperture


The view factor for a point source at some distance d above the center of a detector with a rectangular
aperture with dimensions a × b is [Gossman et al. 2010, 2011]
 
1 (a/d)(b/d)
Pv (a/d, b/d) = arcsin  . (7.85)
π [(a/d)2 + 4][(b/d)2 + 4]

The view factors for rectangular apertures are shown in Fig. 7.17. For case of a square aperture with
dimension a, Eq. (7.85) reduces to

1 (a/d)2
Pv (a/d) = arcsin . (7.86)
π (a/d)2 + 4

Of more utility is the case when the point source is a distance d above a corner of a rectangular aperture
with dimensions a × b. For this case, the view factor is one-quarter that of Eq. (7.85) with a → 2a and
Sec. 7.4. Geometric Effects: View Factors 271

source

3 2 c

4 1 b

e a

Figure 7.18. Calculation of the view factor for a point


source offset from a rectangular detector aperture (solid
Figure 7.17. The view factor for a point source over the lines) when the source, a distance d above the aperture
center of a rectangular aperture as calculated by Eq. (7.85). plane. With Eq. (7.87) the view factor for the aperture is
Data points are Monte Carlo calculated values using MCNP6 Pv1 = Pv1+2+3+4 − Pv2+3 − Pv3+4 + Pv3 , where the superscript
[2013]. is the union of indicated rectangular regions.

b → 2b. The result is  


1 (a/d)(b/d)
Pv (a/d, b/d) = arcsin  . (7.87)
π [(a/d)2 + 1][(b/d)2 + 1]
With this result the view factor can be calculated for the point source located above any point in the aperture
plane! If the source is above the aperture, then a perpendicular line extending from the source to the detector
divides the aperture into four smaller rectangular apertures.
Likewise if the source is not above the aperture, the aperture view factor can be found by adding and
subtracting the view factors for each rectangular region, each of which has the source over a corner. See
Fig. 7.18 for an example. Note, however, that radiations can now enter the side of the detector if the
source is offset from the detector aperture, thereby confusing the view factor situation altogether. Hence,
an additional calculation is needed to account for radiations entering into the side of the detector.
Approximation Method for the View Factor: Under the condition that the point source is sufficiently
far from the detector aperture, and the dimensions of the aperture are similar (a  b), the view factor can
be approximated by replacing the rectangular aperture by a circular one with the same area. Hence, the
aperture area A = ab = πã2 from which the equivalent aperture radius ã is obtained. Then, from Eq. (7.82)
the view factor is * + * +
1 d 1 d
Pvapprox
 1−  = 1−  , (7.88)
2 d2 + A/π 2 d2 + ab/π
where A is the projected area of the detector aperture. Typically, the distance d should be at least equal
to the sum of the aperture’s vertical and horizontal dimensions. Notice that once again Pv depends only on
dimensionless ratios a/d and b/d. Comparison of Eq. (7.85) with Eq. (7.88) shows that if a/d is no greater
than ±40% of b/d, then Pvapprox overestimates Pv by less than 4%.
272 Source and Detector Effects Chap. 7

Example 7.3:
A gas-filled detector with a 3-inch × 2-inch aperture is placed 3 inches away from a 137 Cs source for a
radiation measurement. The source is on the detector axis. What is the solid angle subtended by the NaI:Tl
detector and the resulting view factor? How does the approximation method compare to the exact results?
Assume no intermediate absorption of the gamma rays.

Solution:
From Eq. (7.85)

(a/d)(b/d)
Ω = 4πPv (a/d, b/d) = 4 arcsin 
[(a/d)2 + 4][(b/d)2 + 4]

(3/3)(2/3)
= 4 arcsin  = 0.568 sr.
[(3/3)2 + 4][(2/3)2 + 4]

The view factor is thus Pv = Ω/(4π) = 0.0452.


The approximate method for Pv is given by Eq. (7.88) so
* +
3
Ω= 4πPvapprox  2π 1−  , = 0.576 sr.
32 + (2)(3)/π

Thus, the approximate method overestimates by about 1.5%.

7.4.2 Isotropic Area Sources


Solid Angle for a Disk Source and a Cylindrical Detector
As shown in Fig. 7.19, a radioactive disk source of radius as is centered and placed a distance d from circular
aperture or radius ad . The planes of both disks are parallel. Decay particles can reach the detector aperture
from any location on the disk source. The source emits radiation isotropically at a rate of S0 particles
per unit area per unit time. The rate at which radiation emitted from a differential area of the source,
dAs = r1 dr1 dθ1 , reaches a differential area on the detector aperture, dAd = r2 dr2 dθ2 , is

S0 (n̂•R) dAs dAd


dN = . (7.89)
4πR3
Here n is a unit vector perpendicular to the source, and the term n̂•R/R is the cosine of the angle between
R and n, namely d/R. Thus,

S0 d dAs dAd
dN = 3/2
. (7.90)
[d2 + r12 + r22 − 2r1 r2 cos(φ1 − φ2 )]

The total emission rate from the radioactive source is N0 = S0 4πa2s . Division of Eq. (7.90) by N0 then gives
differential view factor for radiation from dAs to dAd , i.e.,

1 d dAs dAd
dPv = 2 2
. (7.91)
4π as [d2 + r2 + r2 − 2r1 r2 cos(φ1 − φ2 )]3/2
1 2
Sec. 7.4. Geometric Effects: View Factors 273

Detector
Aperture

Disk
Source ad
Ss Sd
as r2

R
f2
f1 r 1 f1
r1

d
Figure 7.20. The view factor for an axially aligned
Figure 7.19. Geometry used to determine the solid disk source and disk detector apertures as calculated
angle for a disk source and cylindrical detector. with Eq. (7.93).

To obtain the total view factor, the above result must be integrated over all dAs and dAd . Ruby [1994]
expressed the result as a single integral involving Bessel functions of the first kind of order one, namely

ad ∞ dk
Pv exp[−kd]J1 (kas )J1 (kad ). (7.92)
as 0 k

This expression, like previous view factors, can be expressed in terms of dimensionless parameters by defining
kd = k  . Equation (7.92) becomes
 ∞
(ad /d) dk  as ad
Pv (as /d, ad /d) = exp[−k  ]J1 (k  )J1 (k  ). (7.93)
(as /d) 0 k d d

Although this result cannot be evaluated analytically, it is easily evaluated using numerical integration.
Example results are shown in Fig. 7.20.
Ruby [1994], by substituting a truncated series approximation for the Bessel functions in Eq. (7.93),
found
"       #
3 15 : 4 ; 35  6 
Pv  ω 1 −
2 2 2
(ψ + ω ) + ψ + ω + 3ψ ω −
4 2 2 6 2 2 2 2
ψ + ω + 6ψ ω (ψ + ω ) , (7.94)
4 24 64

where ψ = as /d and ω = ad /d. Accuracy increases as the distance between the source and detector increases.
In other words, the accuracy increases as ψ and ω decrease, where the error is < 1% for ψ < 0.2 and ω < 0.5.
Another much more complicated, but perhaps a more accurate approximation to Eq. (7.93) was published
later [Vega-Carrillo 1996, 2005]. However, it turns out that numerous solutions and tables for various
geometries for the disk source/cylindrical detector geometry have been published [Jaffey 1954; Paxton 1959;
Hubbell et al. 1961], offering a simplistic alternative method for arriving at view factors for a disk source.
274 Source and Detector Effects Chap. 7

7.4.3 Monte Carlo Approach to View Factor Angle Calculations


The number of source/detector combinations for which the view factors can be evaluated analytically, or
even approximated, is quite limited. However, Monte Carlo techniques can be easily used to numerically
determine view factors, from simple to very complex geometries. Sources and detector apertures of any shape
and orientation to each other are readily treated. Indeed, the programming effort to numerically evaluate
Eq. (7.93) is far greater than that needed for a Monte Carlo evaluation. Monte Carlo results are shown to
agree well with analytical and experimental results for several examples shown earlier in this section.
More important, all of the examples given in this section have assumed isotropic emissions from the
various sources. However, there are many cases in which the emission is quite anisotropic. For example,
radiation emitted from the outer surface of a shielded source is often proportional to some power of the cosine
of the emission angle with respect to the outward normal to the surface. Similarly, radiation emitted from a
collimated source, such as a beam port of a nuclear reactor, is quite anisotropic. Monte Carlo methods can
treat such cases with little extra effort.

7.5 Geometric Corrections: Detector Parallax Effects


Uncollided gamma rays are exponentially attenuated as they travel through a medium. The probability a
gamma ray makes, at least, its first interaction after traveling a distance x in the detector is, thus,

Pint (x) = 1 − e−μ(E)x , (7.95)

where μ(E) is the total interaction coefficient for gamma rays of energy E in the medium inside the detector.
As a first approximation, Eq. (7.95) describes the ex- Detector Solid
pected fraction of photons that have undergone a single Angle
interaction while traveling a distance x. For a photoelec-
Detector
tric interaction, the photon’s full energy is transferred to
the detector medium less, perhaps, some losses from x- i ii
ray escape events. Compton scattering and pair produc- q1
Source q2 iii
tion lead to partial energy deposition. Equation (7.95)
does not take into account small-angle Compton or in- a
coherent scattering, which usually deposits very little
energy in the detector with the secondary photon con- d1 l
tinuing on in nearly the same direction with almost the d2
same energy. This possibility can be accounted for by
removing incoherent and small-angle Compton scatter- Figure 7.21. A radioactive point source at distance d
1
ing components from the interaction coefficient μ(E) in from the center of the aperture of a cylindrical detector.
Eq. (7.95). Particles entering the detector encounter different mass
Hence, the intrinsic efficiency, as given by Eq. (7.74), thicknesses of the detector medium depending on their
trajectories. Shown by the dotted lines are the three
pertains to the efficiency of the detector to have at least limiting trajectories.
one radiation interaction within the detector volume af-
ter radiation particles have crossed the plane of the detector aperture. Because some events may deposit
energy below the system’s electronic threshold, then Eq. (7.74) and Eq. (7.95) give the best possible efficiency
that can be achieved by the detector.
Consider the situation of Fig. 7.21, depicting a cylindrical detector of radius a and length l. The radiation
source is placed at distance d1 from the center of the aperture of the cylindrical detector. However, the
source is also at distance d2 from the exit aperture of the detector. The interaction probability of gamma
rays entering the aperture at angle θ1 is zero. Gamma rays entering the detector at angles between θ1 and
Sec. 7.5. Geometric Corrections: Detector Parallax Effects 275

θ2 have a probability of interaction in the range

μ(E)l
0 ≤ p(x) ≤ 1 − exp − ,
cos θ2
while those entering between θ2 and 0◦ have an interaction probability in the range

μ(E)l
1 − exp − ≥ p(x) ≥ exp[−μ(E)l].
cos θ2

Although Eq. (7.74) indicates that I is constant for all values of θ ∈ [0, θ1 ] because all source particles
emitted in this range reach the detector aperture, parallax effects reduce this efficiency because different
angles of incidence lead to different probabilities that the incident photon will interact within the detector
and lead to a recorded count. A measured efficiency is only reliable for a single geometry. Parallax effects
change the efficiency as the geometry is scaled as by, for example, altering the distance between the source
and detector.
The intrinsic efficiency is determining by both the view factor Pv , the probability a source particle
is emitted toward the detector aperture, and the probability that such particles interact in the detector
upon crossing the aperture. For gamma rays and neutrons, the interaction probability is described by the
exponential dependence of Eq. (7.95). The number of particles interacting within the detector divided by
the number of particles crossing the detector aperture gives the intrinsic efficiency of the detector. If one
assumes a point isotropic source and that any interaction results in a detectable signal, the intrinsic efficiency,
modified to account for the interaction probability p(x) in the detector, is given by
 θ  2π  θ
1 1
r2 (1 − exp [−μ(E)l(θ)]) sin θ dθ dφ (1 − exp [−μ(E)l(θ)]) sin θ dθ
4π r2

I = 0
  2π
0
= 0
θ . (7.96)
1 1 θ 2 sin θ dθ
r sin θ dθ dφ 0
4π r2 0 0

For the cylindrical case shown in Fig. 7.21, the modified intrinsic efficiency is,
    θ1   
1 θ2
μ(E)l μ(E)(a cos θ − d1 sin θ)

I = 1 − exp − sin θ dθ + 1 − exp − sin θ dθ .
1 − cos θ1 0 cos θ θ2 cos θ sin θ
(7.97)
This result cannot be evaluated analytically and numerically methods must be used. Note that most often a
detector is operated with a discriminator level set to reduce (or eliminate) electronic noise and background
radiations. Consequently, the lower level discriminator (LLD) rejects electronic signals that fall below the
set threshold, thereby producing a lower intrinsic detector efficiency than predicted in Eq. (7.97).
The detection efficiency for charged particles is usually adequately described by Eq. (7.74); however,
parallax clipping can yield a measured efficiency that is lower than the theoretical treatment, another con-
sequence of the signal discrimination level. As shown in Fig. 7.22, an alpha-particle point source subtends a
solid angle Ω defined by distance d and aperture radius a. However, alpha particles deposit energy through
ionization along their straight-line trajectories, and sufficient energy must be deposited within the detector
to produce a signal above the LLD setting. At large angles from the detector axis, alpha particles can strike
the detector wall before depositing sufficient energy and hence avoid detection. Suppose the average ioniza-
tion required to produce a measurable signal requires a transit length in the detector of ≥ h. Consequently,
the solid angle that defines intrinsic efficiency, denoted Ω in Fig. 7.22, is defined by the virtual aperture
a = a − h sin θ .
276 Source and Detector Effects Chap. 7

Detector

Detector
Aperture

Particle W W'
Source
q'
a' a

}
d g

Figure 7.22. A radioactive point source of alpha particles at distance


d from the center of the detector aperture. The energy deposited in the
detector depends on the emission angle from the axis. Ω is the solid angle
determined by d and the aperture radius a from Eq. (7.81). The distance h
represents the transit length that a particle must travel to deposit enough
energy for detection. Consequently, the actual solid angle for detection,
Ω , is determined by a = a − h sin θ  and the distance d.

7.5.1 Attenuation and Scattering Effects Outside the Detector


X and Gamma Rays
The determination of a detector’s response is complicated when absorption and attenuation in the envi-
ronment around the detector are considered. Gamma rays emitted towards a detector may be scattered
away from the detector or otherwise interact in the intervening air. For large distances between the source
and detector, the air attenuation may be significant, although parallax effects are greatly reduced. The
attenuation length of gamma rays, defined as the mean-free-path length, is given by 1/μ(E) and is shown in
Fig. 7.23 for different air temperatures at sea level. Such far-field measurements are also made more complex
by photons scattered into the detector from the air and other objects around the detector. Corrections for
such skyshine, roomshine, groundshine, etc., generally require transport analyses.
Gamma-ray attenuation is most pronounced in air and in the source and detector encapsulations for low-
energy photons. Almost all radiation detectors are in sealed packages. Gas detectors are sealed within a gas
chamber, scintillators are typically hermetically sealed in a reflecting cannister, and semiconductor detectors
are sealed in light-tight encapsulation to reduce electromagnetic noise. Also, many types of semiconductor
detectors are chilled to low temperatures, thereby requiring isolation in vacuum cannisters to prevent icing
and convective warming. In all of these packaging cases, low-energy x rays and gamma rays can be attenuated
as they pass through the container towards the detecting medium.

Alpha Particles
Corrections for alpha-particle (and other heavy charged particle) detectors can be more complicated than
just parallax effects. Recall that charged particles deposit energy through Coulombic interactions along their
straight-line trajectories. They lose energy as they travel through any material between their emission points
and the sensitive volume of the detector.
Sec. 7.5. Geometric Corrections: Detector Parallax Effects 277

Figure 7.23. Gamma-ray attenuation lengths, 1/μ(E), in air as a function of energy and temperature at sea level.
Calculated values based on data in the Radiological Health Handbook [1970].

In Fig. 7.24 are shown two cases for a gas-filled detector having a thin window for the aperture. Such
windows are commonly fabricated from aluminized boPET, thereby allowing energetic alpha particles to
pass through to the detection gas. In the case of Fig. 7.24(a), the alpha-particle point source is placed such
that the range of the alpha particles can reach any location on the detector aperture. The view factor is
determined by the solid angle Ω subtended at the source by the aperture. As discussed earlier, because of
parallax effects, the actual solid angle that allows alpha particles to deposit energy above the discriminator
setting is Ω < Ω. Note that energy loss per unit distance (−dE/dx) is typically higher in the boPET than
the medium between the source and detector, thereby strongly influencing Ω .
In the case of Fig. 7.24(b), the alpha-particle point source is placed such that the range of the alpha
particles is too short to reach all locations on the detector aperture. Consequently, the aperture radius a
does not determine the solid angle within which particles can reach the aperture. Instead, the solid angle
Ωs is determined by a smaller effective as , where as is the greatest radius inside of which the alpha particles
have enough energy to reach the detector. Again, due to parallax and energy loss in the window, the actual
solid angle that allows alpha particles to deposit energy above the discriminator setting is Ω .
In both cases shown in Fig. 7.24, use of Ω to correct the count underestimates the source strength. To
determine the correct emission rate, the correct solid angle to use is Ω , which accounts for both parallax
and window energy-loss effects. The correction is further complicated by the fact that energy deposition by
alpha particles is defined by the Bragg ionization curve, in which −dE/dx is not constant. Hence, the length
h, the minimum distance the alpha particle must travel within the detector to be detected, is not a constant
value.
A common method to reduce solid angle and parallax effects for alpha particle measurements is to highly
collimate the alpha-particle source. As a result, the count rate diminishes, thereby requiring significantly
longer measurement times. Also, energy dissipation in the intermediate medium (typically air) can be elimi-
nated by placing the alpha particle source and detector in a vacuum chamber, a measurement method usually
used for alpha-particle spectroscopy with a semiconductor detector, but not with a gas-filled detector.9

9 The gas pressure inside a gas-filled detector can cause the boPET window to expand like a balloon if operated in vacuum,
further complicating the calculation of a correction factor.
278 Source and Detector Effects Chap. 7

Detector t Detector

Ra
t

Source Source
W W' W Ws W'
a'
q' h

}
a' a as
a

h
}

d g d g

(a) (b)
Figure 7.24. In (a) the range of the alpha particle is greater that the longest distance to
the outer boundary of the detector aperture, whereas in (b) the range of the alpha particle
is shorter than this distance. Note that Ω is defined by the detector aperture, Ωs is defined
by the maximum range that the alpha particles can reach the detector aperture, and Ω
is defined by the required transit length that a particle must pass through to still deposit
enough energy for detection.

Beta Particles
Because beta particles, as they give up energy to the ambient medium, travel in very tortuous trajectories,
the above discussion for heavy charged particles does not apply. As discussed in Section 7.2.2, parallax
effects, along with source reflection, air and aperture attenuation, and source encapsulation effects can all
be treated by using a single Monte Carlo simulation. There are no simple methods.
Neutrons
In many neutron experiments, the neutrons travel through air from their source to a detector. Thermal
neutrons, in particular, can undergo significant air scattering, primarily by the nitrogen in air. For example,
consider thermal neutrons produced in a reactor that travel down a reactor beam port to some experimental
area. Such neutrons have a Maxwellian energy distribution characterized by a neutron temperature T and
a thermal-averaged total interaction coefficient (or macroscopic cross section), as given by [Lamarsh 1966],
namely 

π To
Σt = Σt (Eo ) . (7.98)
2 T
Here Eo is a reference energy (usually 0.0253 eV) and To is a reference temperature (usually taken as 293
K).10
For dry air at STP, Σ(Eo ) is 5.01 × 10−4 cm−1 . Thus, the average distance thermal neutrons, with
T = To , travel before they interact in air is λt = 1/Σt = 2.00 m. This result shows that for every 2 m of
neutron travel in air, the fraction that interact is 1 − e−1 = 0.63. To avoid such losses, sometimes a beam
port is fitted with a long polyethylene tube inflated and sealed with a non-interacting gas, such as 4 He, or
other canister containing a vacuum or 4 He.

10 The most probable neutron energy in a Maxwellian flux distribution with a neutron temperature To is Eo = 0.0253 eV.
Problems 279

PROBLEMS
1. A thin layer of a radioisotope that emits 4.13-MeV, 5.1-MeV and 6.95-MeV alpha particles is electro-
plated on an iron substrate opposite and alpha-particle detector. What fraction of the alpha particles
of each energy emitted towards the substrate are reflected back towards the detector? How would one
distinguish alpha particles emitted directly towards the detector from those that are reflected from the
substrate?
2. Plot the backscatter coefficient for monoenergetic electrons from an iron target for energies between 0.1
and 10 MeV.
3. An 241 Am alpha-particle source is placed in a 2π counter which has a dead time of 30 μs. The source
was prepared with a 4-mm diameter, 50-angstrom thick plated deposit upon a 1-mm Ni backing. The
lower level discriminator (LLD) is set to 100 keV. What is the expected count rate, per source particle,
in the detector?
4. A 137 Cs disk source of 1-cm radius is placed and centered 25 cm away from a 3-in × 3-in NaI:Tl detector.
Determine the fraction of gamma rays that intersect the detector aperture.
5. An 116m In foil is activated in a nuclear reactor to use as a source to measure the dead time of a gas-filled
proportional counter. Radiation measurements are performed at set time intervals, each measurement
being 10 sec long, with the following results:
116m
Data for dead-time determination for an In foil source.
T (min) 0 54 108 163 216 270

Counts 331204 260509 182493 114217 65323 35034

T (min) 324 378 432 486 540 594

Counts 18302 9308 4689 2402 1197 604

(a) Use the dead-time decay measurement method of Eq. (7.68)-Eq. (7.69) to find the detector dead
time. (b) Use the dead-time decay measurement method of Eq. (7.71) to find the detector dead time.
(c) Compare the results and discuss.
6. A radiation measurement is conducted in air for a 137 Cs source with a 5-in × 5-in NaI:Tl detector at a
distance of 100 meters. Estimate the fraction of unscattered gamma rays that reach the detector.
7. An 241 Am alpha-particle source is centered and placed 3 mm away from the circular aperture of a
gas-filled proportional counter. The aperture is 5.04 cm in diameter and is composed of 0.4 mg cm−2
boPET. The experiment is conducted at sea level and at 30◦ C. Assume that the alpha particle must pass
through at least 2.5 mm of gas in the detector to be recorded. Radiation measurements are performed
for 3 min each. After each measurement, the source is moved backwards by 2.5 mm, followed by a new
measurement, resulting in the tabular data shown below.
Data for the determination of alpha-particle range.

D (mm) 3 5.5 8 10.5 13 15.5 18 20.5

Counts 237170 224568 210324 193868 176166 159315 142533 125979

D (mm) 23 25.5 28 30.5 33 35.5 38 40.5

Counts 109079 91118 73509 54969 36693 18363 1283 1


280 Source and Detector Effects Chap. 7

(a) After correcting for equivalent air thickness of the window, plot counts versus range.
(b) Based on the subtended solid angle, correct for counts per measurement and plot atop the previous
graph. Determine source strength. Discuss features.
(c) Using the virtual aperture, correct the counts and plot atop the previous graph. Determine source
activity. Discuss the features.

REFERENCES
BAERG, A.P., “Variation on the Paired Source Method of Measur- MARTIN, G.R., “The Estimation of the Resolving Time of a Count-
ing Dead Time,” Metrologia, 1, 131–133, (1965). ing Apparatus,” Nucl. Instrum. Meth., 13, 263, (1961).
BALTAKMENS, T., “A Simple Method for Determining the Maxi- MCGREGOR, D.S. AND J.K. SHULTIS, “Reporting Detection Effi-
mum Energy of Beta Emitters by Absorption Measurements,” ciency for Semiconductor Neutron Detectors, A Need for a Stan-
Nucl. Instrum. Meth., 82, 264–268, (1970). dard,” Nucl. Instrum. Meth., 632A, 167–174, (2011).
CRAWFORD, J.A., “Theoretical Calculations Concerning Back- MCNP6, MCNP6 User’s Manual, LA-CP-13-00634, Los Alamos
Scattering of Alpha Particles,” in The Transuranium Elements, National Laboratory, 2013.
G.T. Seaborg, J.J. Katz, W.M. Manning, Eds., Vol. 2, New York:
McGraw-Hill, 1949. MÜLLER, J.W., “Dead-Time Problems,” Nucl. Instrum. Meth.,
112, 47–57, (1973).
DERUYTTER, A.J., “Evaluation of the Absolute Activity of Alpha
Emitters and of the Number of Nuclei in Thin Alpha Active MÜLLER, J.W., “On the Evaluation of the Correction Factor
Layers,” Nucl. Instrum. Meth., 15, 164–170, (1962). μ(ρ , τ  ) for the Periodic Pulse Method,” Report BIPM-76/3,
Bureau Int. des Poids et Mesures, Sévres, 1976.
EVANS, R.D., The Atomic Nucleus, New York: McGraw-Hill,
1955. NCRP, “A Handbook of Radioactivity Measurements Procedures,”
Report 58, 2nd Ed., Bethesda, Maryland: NCRP, 1985.
FAIRSTEIN, E., ET AL., “IEEE Standard Test Procedures for Ger-
manium Gamma-Ray Detectors,” IEEE Std 325-1996, NIDC, PAXTON, F., “Solid Angle Calculation for a Circular Disk,” Rev.
IEEE, 1996. Sci. Instrum., 30, 254–258, (1959).

GOSSMAN, M.S., A.J. PAHIKKALA, M.B. RISING, AND P.H. MC Radiological Health Handbook, Rev., Rockville, MD: U.S. Depart-
GINLEY, “Providing Solid Angle Formalism for Skyshine Calcu- ment of Health, Education, and Welfare, 1970.
lations,” J. Appl. Clin. Med. Phys., 11, (4), 278-282, (2010). ROSSI, B.B. AND H.H. STAUB, Ionization Chambers and Coun-
GOSSMAN, M.S., A.J PAHIKKALA,M.B RISING, P.H. ters, New York: McGraw-Hill, 1949.
MCGINLEY,“Letter to the Editor,” J. Appl. Clin. Med. Phys., RUBY, L., “Further Comments on the Geometrical Efficiency of
12, (1), 242–243, (2011). a Parallel-Disk Source and Detector System,” Nucl. Instrum.
HUBBELL, J.H., R.L. BACH, AND R.J. HERBOLD, “Radiation Field Meth., A337, 531–533, (1994).
From a Circular Disk Source,” J. Res. National Bureau of Stan- TABATA, T., R. ITO, AND S. OKABE, “An Empirical Equation for
dards, 65C, 249–264, (1961). the Backscattering Coefficient of Electrons,” Nucl. Instrum.
HUTCHINSON, J.M.R., C.R. NASS, D.H. WALKER, AND W.B. Meth., 94, 509–513, (1971).
MANN, “Backscattering of Alpha Particles from Thick Metal VEGA-CARILLO, H.R., “Geometrical Efficiency for a Parallel Disk
Backings as a Function of Atomic Weight,” Int. J. Appl. Rad. Source and Detector,” Nucl. Instrum. Meth., A371, 535–537,
Iso., 19, 517–522, (1968). (1996).
JAFFEY, A.H., “Solid Angle Subtended by a Circular Aperture at VEGA-CARILLO, H.R., Erratum to “Geometrical Efficiency for
Point and Spread Sources,” Rev. Sci. Instrum., 25, 349–354, a Parallel Disk Source and Detector,” Nucl. Instrum. Meth.,
(1954). A538, 814, (2005).
KAPLAN, I., Nuclear Physics, Reading: Addison-Wesley, 1962. VINCENT, C.H., Random Pulse Trains, Their Measurement and
KUZMINIKH, V.A. AND, S.A. VORBIEV, “Backscattering Coeffi- Statistical Properties, IEE Monograph Series 13, London: Peter
cients Calculations of Monoenergetic Electrons and Positrons,” Peregrinus, 1973.
Nucl. Instrum. Meth., 129, 561–563, (1975).
ZEIGLER, J.F., J.P. BIERSACK, AND M.D. ZEIGLER, SRIM: The
LAMARSH, J.R., Introduction to Nuclear Reactor Theory, Read- Stopping and Range of Ions in Matter, available through the
ing, MA: Addison-Wesley, 1966. web at www.srim.org, 2013.
Chapter 8

Essential Electrostatics

I happen to have discovered a direct relation between magnetism and light,


also electricity and light, and the field it opens is so large and I think rich.
Michael Faraday

Numerous radiation detectors rely on the current produced by the motion of mobile charges created by
radiation events. Radiation interactions within the detector volume ionize the absorbing medium, thereby
creating mobile point charges, usually referred to as charge carriers (because these particles carry the charge
through the detector). The detector may be a solid, liquid or gas, within which two or more electrodes are
installed. Generally, a voltage is applied to the detector electrodes to move, or drift, the mobile charges
across the detector volume to produce the current.
Electronic detectors range from simple radiation counters to complex radiation spectrometers. The former
are used to indicate the presence of ionizing radiation, whereas the latter can also identify the energies and
types of radiation. In either case, the fundamental physics of current induction formed by mobile charge
carriers applies. Introduced in this chapter are the basic concepts governing charge and current induction in
electronic radiation detectors.

8.1 Electric Field


Consider a point charge of Q coulombs, as shown in Fig. 8.1. The charge itself has electric field lines
emanating from it radially outward (or inward). If a point charge is centered within an imaginary spherical
surface, the electric field lines intersect the surface at right angles (perpendicular), with the imaginary surface
area 4πr2 , where r is the radius of the sphere. Suppose the number of field lines is denoted by N , then the
surface density of field lines becomes N/(4πr2 ) per unit area. It is easy to understand that the electric field
line density decreases with r2 as the spherical surface area increases. The electric field vector (with SI units
of volts/meter or, equivalently newtons/coulomb) at the surface of the sphere is
Q
E= r̂, (8.1)
4πo r2
where r̂ is a unit vector normal to the spherical surface and o is the permittivity of free space  8.854 × 10−12
farads per meter or, equivalently, A s V−1 m−1 . The magnitude of E is
Q cos θ
E = E •r̂ = . (8.2)
4πo r2
Because the field lines are perpendicular to the spherical surface, then multiplication by the area of the
sphere A = 4πr2 gives
Q cos θ Q
EA = 2
4πr2 = . (8.3)
4πo r o

281
282 Essential Electrostatics Chap. 8

Figure 8.1. An imaginary spherical surface Figure 8.2. An irregularly shaped surface sur-
enclosing a point charge at the center. rounding both the spherical surface and the
point charge.

E DSI E = E cosq
E Note that if the charge is positive, then the
electric field lines point outwards (or positive
direction), and if the charge is negative, then
r’
DS cosq
I q the electric field lines point inwards (or neg-
r line segment of ative direction). In either case, Eq. (8.3) is
q irregular surface =DS
r’ I
still correct. From this result it is seen Q/o
is independent of the size of the sphere. If
the imaginary spherical surface is then sur-
r
rounded by an irregularly shaped surface, as
line segment of
sphere surface = DS cosq
I
shown in Fig. 8.2, the product EA can be
shown to still be the same.
Suppose that the sphere of radius r is
expanded to a radius r such that portions
of the new spherical surface lie inside and
outside the irregular surface, as shown in
point
Fig. 8.3. The electric field lines are still or-
charge thogonal to the sphere of radius r . Consider
a small segment ΔSI along the irregular sur-
Figure 8.3. An irregularly shaped surface surrounding both the
spherical surface and the point charge. The spherical surface is face and a small line segment ΔSS along the

expanded to a new radius of r that intersects the irregular surface. spherical surface. The angle between the two
small line segments is designated θ; hence
the length of the line segment on the sphere must be ΔSI cos θ. Notice also that the angle between electric
field vector and the normal vector to the irregular surface is also θ.
Now apply the same argument to a small area segment ΔAI on the irregular surface that intersects the
spherical surface (see Fig. 8.4). The small area formed by projecting ΔAI back onto the spherical surface is
denoted ΔAS . From the previous results for the line segments, the product EΔAI for the irregular surface
becomes ΔAS = EΔAI cos θ for the spherical surface. In the limit as ΔAI → dAI and ΔAS → dAS , the
integration of E cos θdAI over the irregular surface must equal the integration of EdAS over the spherical
Sec. 8.1. Electric Field 283

cosq
E
q
DAI

DAI cosq E = E cosq


E

q
segment of irregular
surface = DAI

r
q

point segment of sphere


charge surface = DAI cosq

Figure 8.4. It can be shown that the electric field normal to the
irregular surface (E⊥ ) is related to the spherical surface by a factor
of cos θ. Similarly, the small area on the irregular surface, ΔAI , is
related to the small area projected onto the spherical surface, ΔAS ,
by a factor of ΔAI cos θ.

surface, which from Eq. (8.3) equals Q/o , i.e.,


 
Q
E cos θ dAI = E dAS = . (8.4)
AI AS o
Thus, the product of the electric field and total surface area always is Q/o regardless of the shape of a
closed surface surrounding a point charge! Because the irregular surface is arbitrary, this also means the
point charge can be anywhere inside this surface. For multiple point charges inside SI , each charge Qi
contributes Qi /o , meaning
% that the total charge is the summation of charges within the surface surrounding
the charges Qtotal = i Qi .
Finally, if n̂ is a unit vector perpendicular to any closed surface S, then E cos θ dAS = E •n̂ dAS and
Eq. (8.4) can be written as

  %
Qi Qtotal
E •n̂ dAS = E •n̂ dS = i
= . (8.5)
AS S o o

This is commonly referred to as Gauss’ Law.1

1 Eq.(8.5), credited to Carl Friedrich Gauss, is actually an application of his Law of Quadratic Reciprocity that he rediscovered
in 1795. This result was actually derived by Joseph-Louis Lagrange many years earlier in 1785.
284 Essential Electrostatics Chap. 8

8.1.1 Alternate Derivation of Gauss’ Law


A more mathematically direct way, although not so insightful, to derive Gauss’ law is to start with the first
of Maxwell’s four equations of electromagnetism, namely

∇•D(r) = ∇• [κo E(r)] = ρV (r), (8.6)

where D(r) is the dielectric displacement, κ is the dielectric constant, and ρV (r) is the volumetric charge
density (coulombs per cubic meter). Usually the dielectric constant is unchanged through a medium, although
not always. Suppose in this example that the charge is in an evacuated space surrounded by a surface. Hence,
κ = 1 and Eq. (8.6) can be rewritten as,
ρV (r)
∇•E(r) = , (8.7)
o
Equation 8.7 is integrated over a closed volume V to obtain
 
1 Qtotal
∇•E(r) dV = ρV (r) dV = . (8.8)
V o V o
Here Qtotal is the total charge contained in the volume V . The remaining volume integral can be converted
to an integral over the surface S of V by using Gauss’ divergence theorem [Riley et al. 2006] to obtain

Qtotal
E •n̂ dS = , (8.9)
S o
where n̂ is the outward unit normal to the surface S. Equation (8.6), or the alternative form Eq. (8.7), are
usually referred to as Gauss’ law in differential form, while Eq. (8.9) is Gauss’ law in integral form.

8.2 Electrical Potential Energy


An electric field causes mobile charges to move, hence an electric field does work on a mobile charge. The
work required to move the particle from position r1 to position r2 is given by
 r2  r2
W = F dl =
• F cos θ dl, (8.10)
r1 r1

where F is the force vector applied to the particle, dl is a differential length along the direction of travel,
and θ is the angle between these two vectors. Coulomb’s law states that the force on a particle at r with
charge q  from a second particle at r with charge q is
QQ (r − r ) QQ
F= with magnitude F = , (8.11)
4πo |r − r |3 4πo r2
where r is the distance between the charges.
Consider the electric field of a point charge Q shown in Fig. 8.1. If another point charge Q is placed in
the electric field of the first charge Q, then the electric field of Q exerts a force on Q , and the electric field
of Q exerts an equal force on Q.
In Fig. 8.5, a single charge Q is moving in the electric field of a second charge Q from position r1 to
position r2 across the field lines of Q. In the limit of decreasing angles between field lines, Δω → dω, Δl → dl,
Δr → dr, and θ1 = θ2 = θ. From Fig. 8.5, the relationship between the differential distance traveled dl and
the differential change in distance between the charges dr is

cos θ dl = dr. (8.12)


Sec. 8.2. Electrical Potential Energy 285

Substitution of Eq. (8.12) into Eq. (8.10) then yields the work done on the point charge Q as it moves
from some point r1 to r2 ,
 r2  r2  
1 QQ QQ 1 1
W = F dr = 2
dr = − . (8.13)
r1 r1 4πo r 4πo r1 r2

This result shows that the path taken from r1 to r2 is imma-


terial, but instead only the change in radial distance from
Q determines the work done. In other words, it is only the
starting and ending locations that determine the total work
performed on the charge moving in the electric field.2 F
The potential energy of a particle with charge Q located
a distance r away from another particle of charge Q is rep- Dw
resented by Dr
1 QQ q1 r1
U= . (8.14) Dl
4πo r q2
Q'

Suppose that the particle with charge Q is surrounded by
n particles with charge Qi at distance ri from the particle r2

with charge Q . The total potential energy exerted on the
particle with charge Q from the collective electric fields of
Q
the surrounding particles is
 
Q  Qi
n
Q Q1 Q2 Q3 Qn
U= + + + ... + = . Figure 8.5. Depiction of charge Q moving
4πo r1 r2 r3 rn 4πo i=1 ri through the electric field of charge Q.
(8.15)
The potential energy of an individual charged particle is useful, and is important for understanding
signal formation within an electronic radiation detector. However, it is more common to use the general
term potential, which is defined as the potential energy per unit charge,

1  Qi
n
U
V = = , (8.16)
Q 4πo i=1 ri

and is expressed in units of volts (or joules per coulomb). Note that the potential is no longer dependent
upon the “test” charge Q .3 The force exerted upon Q may also be expressed in terms of the electric field,
produced by one or more point charges, in which F = Q E. Substitution of q  E into Eq. (8.13) and division by
Q gives the potential difference between two points within the electric field. Hence, the potential difference
between arbitrary locations a and b is
 b  b
Vab = ΔV = E •dl = E cos θ dl. (8.17)
a a

2 The path independence is a consequence that F of Eq. (8.11) is given by the gradient of a scalar field potential, i.e.,
 
QQ
F=∇ .
4πo r
As a result ∇•F = 0. Force fields with this property are called conservative force fields.
3 The normalization unit charge Q is that of a free electron, qe , such that Q = qe N  where N  is an integer. For a single
electron, N  must equal unity. Other charges are therefore integer representations of qe , namely, Qi = qe Ni .
286 Essential Electrostatics Chap. 8

In summary, Eq. (8.17) is the voltage that an experimenter would measure between two points (a and b)
within an electric field. The work done on a unit test charge moving from some point a to another point b
in the electric field is Q Vab .

8.3 Capacitance
Consider the arrangement depicted in Fig. 8.6. Two conductive plates, separated by a distance d, have
equal, but opposite, charges. An electric field is produced between the plates by the charges on the plates.
The positively charged plate (or terminal) has a voltage V1 and the negatively charged plate has a voltage
V2 . The capacitance of the two plates is defined as the ratio of the charge magnitude on either plate to the
magnitude of the potential difference between the plates,
 
 Q 
C=  . (8.18)
ΔV 

If ΔV is taken as the applied voltage V between the electrodes, then the above definition gives the important
relation
CV = Q (8.19)
The SI unit for capacitance is the farad (one coulomb per volt). The reader should understand that the
charge stored in a capacitor has a summed positive charge on one terminal and an equal summed negative
charge stored on the opposite terminal; hence, a capacitor with stored charge Q actually has +Q on one
terminal and −Q on the other terminal.
Many radiation detectors use a voltage applied between two conductive terminals. Of these de-
tectors, the parallel plate configuration, similar to that shown in Fig. 8.6, is the simplest and easi-
est to understand. The finite area of either plate has a charge of magnitude Q. Hence, there is an
average charge magnitude per unit area, defined as a surface charge density σ. Assume that there
is a vacuum between the conductive plates and that the conductive plates have equal areas A and
are separated by a distance d, then the magnitude of the electric field between the parallel plates is
Q+ σ Q
V1 + + + + + + + + + + + E= = . (8.20)
o o A

E d From Eq. (8.17), the voltage difference between the plates is

V2 - - - - - - - - - - - V = Ed =
Qd
. (8.21)
Q- o A

Figure 8.6. Two conductive plates separated Substitution of Eq. (8.21) into Eq. (8.19) yields the capacitance
by distance d have equal, but opposite, charges
stored upon them. The cumulative charges pro- A
duce an electric field, with a voltage of V1 at the C = o . (8.22)
positive charge terminal and a voltage V2 at the d
negative charge terminal.
A radiation detector has a radiation absorbing medium, such
as a gas or semiconductor, between the conductive electrodes. The permittivity of the radiation absorbing
material must be substituted into Eq. (8.22), which is accomplished by multiplying o by the dielectric
correction constant κs of the radiation absorbing material,

A
C = κs  o . (8.23)
d
Sec. 8.4. Current and Stored Energy 287

Note that the electric field, voltage and charge terms are not necessary to define capacitance; hence, the
capacitance is dependent only upon the device dimensions and permittivity of the insulating material between
the electrodes.
Many advanced detector designs do not have simple parallel plate geometries, and many detectors are
designed to reduce capacitive effects. Gas filled detectors are often designed in a coaxial configuration with a
single anode wire through the center with a much larger cylindrical outer conductive cathode shell. There are
detector designs with numerous anodes (or cathodes), some detectors have concentric spherical electrodes,
and many detectors have a variety of different electrode shapes. Because Eq. (8.23) applies only to simple
planar geometries, capacitance for these other detector geometries must be found by deriving a fundamental
form of Eq. (8.19) for each particular geometry of interest.

8.4 Current and Stored Energy


Capacitors are generally used as charge storage devices, and these charges are transported to a capacitor
through an electronic circuit. Consider the movement of charge ΔQ to a capacitor in some time interval
Δt. The current I is defined as the amount of charge transported divided by the time taken for the charge
movement, i.e.,
ΔQ ΔV
I= =C . (8.24)
Δt Δt
The rate at which charge flows to a capacitor, or other electronic components may not be constant in time;
hence, the instantaneous current is defined as
dQ dV
I= =C . (8.25)
dt dt
Charges flowing to a capacitor build up the charges on one side of the capacitor, which causes charges of the
opposite polarity to accumulate on the opposing electrode. Consequently, work is performed to accumulate
the change in charge ΔQ in the capacitor. From Eq. (8.10), the work to increase the electrode charge by dq

q
dW = dq E cos θ dl = V dq = dq. (8.26)
C
where V is the magnitude of the voltage on the capacitor at a time when the accumulated charge is q. If
no charge is initially stored on the capacitor, Eq. (8.26) is integrated to find the total work performed to
accumulate charge Q on the capacitor, i.e.,
 W  Q
q Q2
W = dW = dq = . (8.27)
0 0 C 2C

With Eq. (8.19), the work performed to store Q, which is also the energy stored by the capacitor, can be
expressed as
Q2 QV CV 2
W = = = . (8.28)
2C 2 2
This result is important for electronic radiation detectors. Suppose a radiation interaction occurs within an
electronic radiation detector, on which a voltage V0 is applied across the detector terminals. The mobile
charges created by the radiation event are caused to move (or drift) through the detector. Positive charges
drift towards the negatively charged electrode and negative charges drift towards the positively charged
electrode. As these charges separate, they form a small, time-dependent electric field of opposite polarity to
that of the electric field applied to the detector. As a result, a small change in voltage appears between the
288 Essential Electrostatics Chap. 8

iB
iA B B
iC
QA C C
A Q A
VA = 0 V’
A =1

D
iD D

iE
Vr E
V’r
E

Figure 8.7. A point charge Q is placed Figure 8.8. The point charge is re-
in the vicinity of grounded conductive moved and a potential equal to unity
surfaces, and produces image charges is applied to A. All other electrodes re-
on those surfaces. main grounded.

electrodes caused by the electric field of the drifting charges. Hence, stored energy is expended to move the
charges, and the energy expended to move the charges can be measured as a change in current or voltage
that, typically, is performed by an externally connected circuit.
Charges moving in a detector cause current to flow in an externally connected circuit through a process
called induction. In other words, mobile charges moving in the detector cause electron current to flow in
the circuit externally connected to the detector. The change in electron current can be measured directly,
commonly referred to as current mode operation, or it can flow to a capacitor in the external circuit and
be stored, thereby providing a measure of the voltage change as defined by Eq. (8.19). This change in
voltage ΔV , or voltage pulse, signals the occurrence of a radiation interaction event in the detector. Such
measurements are referred to as pulse mode operation.

8.5 Basics of Charge Induction


Many radiation detectors are based on the principle of charge induction, whereby moving point charges work
to induce a current in an external circuit. The detector itself is a capacitor, and charges moving in the
detector cause current flow to or from the device terminals or electrodes. The charge or current induced on
any electrode can be found through Shockley’s or Ramo’s method (both methods are essentially the same)
[Ramo 1939; Shockley 1938].
Consider a single point charge Q situated at position rq in a vacuum within which there are an arbitrary
number of grounded conducting surfaces, as depicted in Fig. 8.7. The point charge Q will cause electrons
on the surrounding conductive surfaces to change in position. If Q is negative, then the surface electrons
will be slightly repelled, while if positive, slightly attracted to the surface. The overall effect is to have the
apparent appearance of an image charge of opposite sign on the conductive surface. Suppose the goal is
to determine the induced current and induced charge produced upon electrode A by the point charge Q,
thereby producing an image charge of QA on the electrode. Perhaps the other electrodes are also affected,
but it will shortly be seen to be of no consequence to this derivation. Surround the point charge Q by a
small equipotential conducting sphere. From Gauss’ law one has
 
∂V Q
E n̂ ds =
• ds = , (8.29)
sph sph ∂n  o
Sec. 8.5. Basics of Charge Induction 289

where n̂ is the outward unit normal to the surface and ∂V /∂n denotes ∇V •n̂.
Because there are no charges in the vacuum bounding the electrodes and the small sphere, the electrostatic
field is given by Laplace’s equation
∇2 V (r) = 0, r ∈ all space outside the conducting surfaces. (8.30)
The boundary conditions needed to specify a unique solution of Eq. (8.29) are V (r) → 0 as |r| → ∞ and by
the voltages on the electrodes. The voltage on the small imaginary sphere is denoted by Vr = V (r).
Now for the same set of electrodes with the charge Q removed, electrode A is given a voltage VA with
the other electrodes still grounded, as shown in Fig. 8.8. The new electrostatic field, V  (r), is described by
∇2 V  (r) = 0, (8.31)
with boundary conditions specified by the voltage on all surfaces. The voltage at r at the surface of the
imaginary sphere is now Vr = V  (r). Apply Green’s theorem [Riley et al. 2006] to all surfaces, namely
 
 2 2  ∂V ∂V 
[V ∇ V − V ∇ V ]dv = V −V ds. (8.32)
vol S ∂n ∂n
Here the surface integration is over all electrode surfaces, the imaginary surface, and the surface at infinity,
and the volume integration is over all space bounded by all the surfaces. From Eq. (8.30) and Eq. (8.31) the
left-hand side of Eq. (8.32) is seen to vanish. On the right-hand side the surface integral at infinity vanishes
because V (r → ∞) = V  (r → ∞) = 0. The surface integrals around all grounded electrodes also have the
potential V and V  equal to zero, hence, the right side of Eq. (8.32) vanishes for these electrodes. Thus, only
the surface integrals around the charged electrode A and around the small sphere remain, and Eq. (8.32)
reduces to [Ramo 1939],
   
∂VA ∂VA ∂Vr ∂Vr
VA ds − VA ds + Vr ds − Vr ds = 0. (8.33)
SA ∂n SA ∂n sph ∂n sph ∂n

From Gauss’ law the first integral equals QA /o , where QA is the image charge on electrode A. Similarly,
the third integral equals Q/o. The second term vanishes because VA = 0. From Eq. (8.29), the fourth
integral vanishes because there is no charge inside the small imaginary sphere. Thus,
QA Q Vr
VA + Vr = 0 or QA = −Q . (8.34)
o o VA
From this result the induced current produced by the point charge in Fig. 8.7, moving in any direction
between the electrodes with vector velocity v = dr/dt, is
dQA Q dVr Q dr Q
IA = =−  = −  ∇Vr (r)• =  E  (r)•v, (8.35)
dt VA dt VA dt VA
where E  (r) is the electric field at point r under the condition that the “potential” at electrode A is set at
VA with all other electrodes grounded.
It is useful to normalize V  (r) by setting VA to one volt, i.e., define Vw (r) ≡ VQ (r)/VA . This normalized
“voltage” Vw is called the weighting potential although it is dimensionless. In terms of this normalized
potential, Eq. (8.34) and Eq. (8.35) are expressed as

dr
QA = −QVw (r) and IA = −Q∇Vw (r)• = QE w (r)•v (8.36)
dt
290 Essential Electrostatics Chap. 8

where the normalized or weighting electric field is E w = E  /VA = −∇Vw . This result can be applied to any
one of the electrodes by setting its potential to one volt and grounding all other electrodes [see also Jen 1941;
Beck 1953]. The results of Eq. (8.36) are significant and important, and are often referred to as Ramo’s
Theorem.4 Hence, for any geometric detector structure, the expected current induction for the electrode tied
to the readout circuit can be found from Eq. (8.36).
One can calculate the weighting potential for practically any electrode configuration by solving Laplace’s
equation (Eq. (8.30)) with the boundary conditions that (1) the contact connected to the readout electronics
is set to unity and (2) all other contacts are grounded (set to zero). Weighting potentials for a few select ge-
ometries are easily calculated by analytical means, while weighting potentials for more complicated electrode
geometries may be calculated by finite difference methods.

8.5.1 Green’s Reciprocation Theorem


Suppose there is an array of M conductors in a vacuum and charges Qi , i = 1, . . . , M are placed on the
conductors to produce potentials Vi , i = 1, . . . , M . Then if these charges are replaced by different charges
Qi , i = 1, . . . , M a different set of potentials Vi , i = 1, . . . , M would result. How are the old charges and
potentials related to the new charges and potentials?
The potential fields are given by ∇2 V (r) = 0 and ∇2 V  (r) = 0 with appropriate boundary conditions.
Equation (8.32) is Green’s theorem and relates V to V  . Because ∇2 V (r) = 0 and ∇2 V  (r) = 0, the left-hand
side of Eq. (8.32) vanishes. Also the integral over the surface at infinity, where both V and V  are zero,
vanishes. Thus, Eq. (8.32) reduces to [Smythe 1989]
M 
 ∂V ∂V 
Vi − Vi dsi = 0,
i=1 Si ∂n ∂n

where Si is a closed surface around electrode i. The V and V  are constant on the surface so Eq. (8.5.1) can
be written as
M  M 
∂V ∂V 
Vi dsi = Vi dsi , (8.37)
i=1 Si ∂n i=1 Si ∂n

which, from Gauss’ law (see Eq. (8.29)), yields the important result


M 
M
Qi Vi = Qi Vi . (8.38)
i=1 i=1

This result is commonly referred to as Green’s reciprocation theorem [for more details, see Jeans 1943; Jackson
1975; Smythe 1989].

8.6 Charge Induction for a Planar Detector


The simplest geometry for a radiation detector that depends on charge induction is the planar device and
consists of two parallel conductors or terminals separated by a radiation absorbing medium. This configu-
ration is often used for simple gas-filled or semiconductor radiation detectors. A voltage is typically applied

4 Although Eq. (8.36) is commonly referred to as “Ramo’s theorem,” the same result was actually published by Shockley in
1938 a year before Ramo’s publication in 1939. Because both Vw and E w are dimensionless, Eqs. (8.36) are dimensionally
correct, although many forget this fact.
Sec. 8.6. Charge Induction for a Planar Detector 291

across the terminals to produce an electric field throughout the radiation absorbing medium. When a ra-
diation interaction occurs within the detector volume, No electron-ion pairs are created. Because of the
electric field across the device, free electrons, with charge −q and positive ions, with charge q drift within
the detector medium toward the conductive surfaces, with negative charges moving towards the anode and
positive charges moving towards the cathode. Both conductive terminals are connected within the same
circuit, as shown in Fig. 8.9.

electron-ion
pairs g-ray
A V+

-
++ -
- + A
++ - -

B
x

0 x1 x0 x2 d
Figure 8.9. Depiction of a planar radiation detector where a gamma ray
is absorbed at location x0 . The figure shows a preamplifier attached to the
positively biased electrode at x = d.
The electrostatic field within the absorbing medium, in the absence of free charges, is given by Laplace’s
equation ∇2 V (r) = 0.5 By picking the x-axis to be perpendicular to the terminals, with the origin at the
grounded terminal, as shown in Fig. 8.9, the potential varies only with x and the potential is given by

d2 V (x)
∇2 V (x) = = 0, (8.40)
dx2
subject to the boundary conditions V (0) = 0 and V (d) = VB . Integration of Eq. (8.40) twice and application
of the boundary conditions to evaluate the two constants of integration yields
VB
V (x) = x. (8.41)
d
The dimensionless weighting potential Vw (x) is obtained by dividing this result by VB or, equivalently,
by setting VB = 1 volt. In either way, for a planar device Vw (x) = x/d. With this weighting potential, the
induced charge in the electrodes is readily calculated.6
In some circumstances, it is important to separately calculate the induced charge contributions from
the electrons and positive ions liberated by radiation. Instances requiring separate treatments may involve

5 Laplace’s equation is simply Poisson’s equation with ρ equal to zero,


ρ
∇2 V (r) = −∇•E(r) = − . (8.39)
κo

6 Some textbooks describe the output of a planar detector with conservation of energy methods. However, the reader is warned
that the conservation of energy approach is generally incorrect, although it may appear to work for special cases. The
consequence of using the conservation of energy approach is especially problematic with semiconductor detectors and should
be avoided.
292 Essential Electrostatics Chap. 8

different charge carrier velocities or different recombination/trapping times for electrons and ions. Such
treatments are covered in later chapters. Here it is assumed that charge carrier velocities and trapping are
of no consequence, so the separate contributions of electrons and positive ions to the induced current can
be determined in a straightforward manner. Consider the situation depicted in Fig. 8.9, where a radiation
interaction event occurs at distance x0 between two electrodes, labeled A and B, separated by a distance of
d. A positive voltage potential is applied at electrode B, such that electrons drift to electrode B and positive
ions drift to electrode A.
The change in the induced charge on electrode B resulting from the total displacement of No charge pairs
moving between the electrodes can be found by using Ramo’s Theorem. Upon integration of the induced
current given by Eq. (8.36), the induced charge on the electrodes ΔQ after the ions have moved from x0 to
x1 and the electrons have moved from x0 to x2 is
 t(x1 )   t(x2 ) 
 
ΔQ = IA (t) dt + IA (t) dt
0 ions+ 0 e−
   
t(x1 )
dr  t(x2 )
dr 
= −qe No ∇Vw dt − (−qe No ) ∇V dt , (8.42)
dt  dt e−
• w•
0 ions+ 0

where qe is the magnitude of the electron charge, t(x1 ) is the time required for the ions to move from
x0 to x1 , and t(x2 ) is the time required for the free electrons to move from x0 to x2 . In this geometry
Vw (r) = Vw (x) = x/d so Eq. (8.42) can be evaluated as follows.
 t(x1 )     t(x2 ) 
dVw dx  dVw dx 
ΔQ = −qe No dt − (−qe No ) dt
0 dx dt ions+ 0 dx dt e−
 t(x1 )   t(x2 ) 
d x dx  d x dx 
= −qe No dt + qe No dt
0 dx d dt ions+ dx d dt −
 x1   x2  0  e 
1   1   
x0 − x1  x2 − x0 
= −qe No dx + qe No dx = qe No + , (8.43)
x0 d ions+ x0 d e− d ions+ d e−

which yields the final result,

x2 − x1
ΔQ|planar = qe No . (8.44)
d

Hence, the total displacement of the free carriers divided by the detector active region width yields the
change in the induced charge measured by the detector. If all of the electrons drift to the positive contact
at x = d and all of the positive ions drift to the negative contact at x = 0, then x2 − x1 = d − 0, and the
induced charge becomes Q = qe No .
Analysis Based on Green’s Reciprocation Theorem
The induced charge can also be found by using Green’s reciprocation theorem as stated by Eq. (8.38).
Consider the two electrodes in the planar device, both of equal dimensions separated by distance d. Two
different situations are now considered. In Case 1, a charge Qo is placed between the plates on an imaginary
infinitely small conductor (labeled conductor 3). Plate A has, as a consequence, an induced charge QA
and plate B has an induced charge QB . The potentials on the electrodes A and B are zero (Case 1). The
induced charges QA and QB are to be determined by Green’s reciprocation theorem. In Case 2 the charge
Qo is removed from imaginary conductor 3 (so that Qo = 0), and placed on electrode B. In both cases the
potentials and resulting induced charges are unknown and are summarized in Table 8.1.
Sec. 8.6. Charge Induction for a Planar Detector 293

Table 8.1. Charge and potential conditions for two electrodes between
which a unit mobile charge (Qo ) is present.
Case 1 (unprimed) Case 2 (primed)
Electrode A B 3 A B 3
Charge QA QB Qo QA Qo 0
Potential 0 0 Vo VA VB Vo

From Green’s reciprocation theorem of Eq. (8.38) for a general electrode problem

Q1 V1 + Q2 V2 + Q3 V3 = Q1 V1 + Q2 V2 + Q3 V3 ,

or rewritten for this specific case,

QA VA + QB VB + Qo Vo = QA VA + QB VB + Q3 Vo .

In the present analysis, VA = VB = Q3 = 0 and the above general relation reduces to

QA VA + QB VB + Qo Vo = 0. (8.45)

Because the sum of the induced charges and the charge Qo , causing the induced charges, must sum to zero,
one also has
QA + QB + Qo = 0. (8.46)
From Eq. (8.45) and Eq. (8.46) the induced charges in Case 1 are found to be
Vo − VB VA − Vo
QA = −Qo and QB = −Qo . (8.47)
VA − VB VA − VB
What does this mean? The charge induced by the test charge on a given electrode is proportional to the
potential difference between the location where the charge originally appeared (in our case, at xo ) and the
opposite electrode. It is a change in the induced charge that causes induced current to flow, and we seek to
find the change in the induced charge as the test charge moves through the space between the electrodes.
With these results, the change in induced charges on the terminal electrodes as the test charge Qo in
Case 1 is moved to a new location between the terminals. The potential on the imaginary electrode in Case
2 changes from Vo to Vn . The change on electrode A is thus
   
V  − VB Vo − VB V  − Vo
ΔQA = −Qo n  − −Q o   = −Qo n , (8.48)
VA − VB VA − VB VA − VB
and the change in the induced charge on electrode B is
   
V  − Vn VA − Vo V  − Vo
ΔQB = −Qo A  − −Q o   = Qo n . (8.49)
VA − VB VA − VB VA − VB

Notice that Eq. (8.48) and Eq. (8.49) have opposite charge signs, hence ΔQA on electrode A is opposite
in sign for ΔQB on electrode B. A knowledge of the equipotential lines between the conductors is needed
in order to apply the results of Eqs. (8.48) and (8.49), otherwise referred to as the weighting potential. As
stated before, the weighting potential can be calculated by solving Laplace’s equation with the electrode of
interest placed at a unit potential while all other electrodes are grounded. Hence, the difference VA − VB
becomes unity, and the normalized potentials Vo and Vn can be determined.
294 Essential Electrostatics Chap. 8

Once again consider the situations shown in Fig. 8.9. Suppose that the electrons move in the positive x
direction to point x2 with potential V  (x2 ) = V2 and the positive ions move in the negative x direction to
point x1 with potential V  (x1 ) = V1 . From Eq. (8.49), the change in induced charge on electrode B, from
both the contribution of the negative electrons and positive ions, is
 
V2 − Vo  V1 − Vo 
ΔQB = −qe No   and + qe No   ,
VA − VB  − VA − VB  +
e ions

where No is the number of electron-ion pairs in motion. A unit negative charge on electrode B would produce
a potential profile described by Eq. (8.41), namely
x
V (x) = −Vo . (8.50)
d
A normalized potential difference within the device is

V (x2 ) − V (x1 ) x2 x1 x2 − x1
= − = . (8.51)
−Vo d d d
This result shows that the potential between the two parallel terminals is simply the displaced distance
divided by d. With the proper charge sign for the ions and electrons, the two contributions to Eq. (8.6) are
 
V2 − Vo  x2 − x0 V1 − Vo  x1 − x0
−qe No   = −qe No and qe No   = qe No . (8.52)
VA − VB  − d VA − VB  +
d
e ions

Addition of these two results and use of Eq. (8.49) yields


x1 − x0 x2 − x0 x2 − x1
ΔQB = −qe No + qe No = qe No .
d d d
This is the same result as Eq. (8.44) obtained by using Ramo’s theorem. With the use of the same
method, it can be shown that the change in the induced charge on electrode A is
x1 − x0 x2 − x0 x2 − x1
ΔQA = qe No − qe No = −qe No .
d d d
Although Ramo’s theorem and Green’s reciprocation relations give the same result for the induced charge,
it is obvious that Ramo’s theorem is considerably easier to use than Green’s reciprocation theorem.

8.6.1 Planar Detector with Stationary Space Charge


Now consider a planar detector in which a stationary uniform distribution of space charge is present as shown
in Fig. 8.10. Such space charge is typical for many semiconductor detector devices. In this case the induced
charge can be found once again from Ramo’s theorem; however, the operating potential must be solved using
Poisson’s equation for electricity.
First, consider Green’s reciprocation theorem for two cases. In Case 1 there is a single mobile charge
Qo placed on a small imaginary electrode and a single stationary charge Qs also on a small imaginary
electrode, both located between electrodes A and B, with potentials Vo and Vs , respectively. Now in Case
2, each charge is independently placed upon electrode A and analyzed. The charges QAo and QBo are the
charges induced by the mobile charge Qo on electrodes A and B, and the charges QAs and QBs are the
charges induced by the stationary charge Qs on electrodes A and B, respectively. The electrode M is the
Sec. 8.6. Charge Induction for a Planar Detector 295

stationary electron-ion
space charge pairs
g-ray
A V+
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + -+ + + + + + + + + +
+ + + + + + + +
++ ++ +- + + + + + + + +
- +
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+++ +++- ++- +
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+
A
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + + B
x

0 x1 x0 x2 d

Figure 8.10. Depiction of a planar radiation detector with a uniform dis-


tribution of positive stationary space charge. The gamma ray is absorbed
at location x0 .

Table 8.2. Charge and potential conditions for two electrodes between which a unit space charge
Qs and a unit mobile charge Qo are present.
Case 1 (unprimed) Case 2 (primed)
Electrode A B M S A B M S
Mobile
Charge QAo , QAs QBo , QBs Qo Qs Qo , QAs QBo , QBs 0 Qs
Charge
Potential 0, 0 0, 0 Vo Vs  ,0
VAo  ,0
VBo Vo Vs
Electrode A B M S A B M S
Stationary
Charge QAo , QAs QBo , QBs Qo Qs QAo , Qs QBo , QBs Qo 0
Charge
Potential 0, 0 0, 0 Vo Vs 
0, VAs 
0, VBs Vo Vs

imaginary electrode at the initial location of the mobile charge and electrode S is the imaginary electrode
at the location of the stationary charge. The Green’s reciprocation conditions for the mobile and stationary
 
charges are summarized in Table 8.2, in which VA0 and VB0 are the potentials produced at electrodes A and
 
B, respectively, by the mobile point charge Qo , and VAs and VBs are the potentials produced at electrodes A
and B, respectively, by the stationary point charge Qs . The induced charges on electrodes A and B, shown
in Table 8.2, have been separated for the stationary and mobile charges.
Green’s reciprocation theorem of Eq. (8.38) is used for this analysis


12 
12
Qi Vi = Qi Vi ,
i=1 i=1

which, upon using values from Table 8.2, expands as


 
QAo VAo + (QAs ×0) + QBo VBo + (QBs ×0) + Qo Vo + Qs Vs + (QAo ×0) + QAs VAs

+

(QBo ×0) + QBs VBs + Qo Vo + Qs Vs = (Qo ×0) + (QAs ×0) + (QBo ×0) + (QBs ×0) +
(Vo ×0) + Qs Vs + (Qs ×0) + (QAo ×0) + (QBs ×0) + (QBo ×0) + Qo Vo + (Vs ×0).
296 Essential Electrostatics Chap. 8

This result simplifies to


 
QAo VAo + QBo VBo + Qo Vo + QAs VAs
 
+ QBs VBs + Qs Vs = 0. (8.53)

The sum of the charge and its resulting induced charges must equal zero, i.e.,

QAo + QBo + Qo = 0 and QAs + QBs + Qs = 0. (8.54)

From Eqs. (8.53) and Eqs. (8.54), the induced charge on electrodes A and B are

Vo − VBo

V  − VBs

QA = QAo + QAs = −Qo   − Qs s  , (8.55)
VAo − VBo VAs − VBs

and 
VAo − Vo V  − Vs
QB = QBo + QBs = −Qo   − Qs As . (8.56)
VAo − VBo VAs − VBs
Now suppose that m space charges are added between the electrodes. The induced charge upon the
output electrode B becomes

VAo − Vo m 
VAs − Vsi
QB = −Qo  −V − Q si 
i
 . (8.57)
VAo Bo i=1
VAsi − VBs i

The observed change in the induced charge upon electrode B if the mobile charge moves from position x0
to a new position xn is
$ /

VAo − Vn  m 
VAs − Vsi
ΔQB = −Qo   − Qsi  i

VAo − VBo i=1
VAsi − VBs i

$ /

VAo − Vo 
m
V  − Vsi Vn − Vo
− −Qo   − Qsi Asi  = Qo  −V .
VAo − VBo i=1 VAsi − VBs i
VAo Bo

This is the same answer as Eq. (8.49)! Hence, it is seen that any space charge does not affect the change in
the induced charge created by the mobile charge. Also notice that the potential change is with respect to the
 
potential distribution that is created by the mobile charge (VAo − VBo ) and not the applied voltage or the
potential distribution created by the numerous m number of stationary charges. As a result, the change in
the induced charge for the planar device, even with stationary space charge present, yields the same result
as given by Eq. (8.44), i.e.,
x2 − x1
ΔQ|planar = qNo .
d
The operating potential is determined, in general, from Poisson’s equation,

ρ(r)
∇2 V (r) = − , (8.58)
s
subject to suitable boundary conditions. For the planar detector V (r) → V (x) and ρ is constant. Thus,
Poisson’s equation becomes
d2 V (x) dE(x) ρ
=− =− , (8.59)
dx dx s
Sec. 8.6. Charge Induction for a Planar Detector 297

where the s = κs o is the permittivity of the detector material. Integration of Eq. (8.59) gives the electric
field as
ρ
E(x) = x + C1 ,
s
where C1 is a constant of integration. For simplicity, it is assumed that the device is fully depleted so that
the electric field vanishes at x = 0 so that C1 = 0.7 Integration once again gives V (x)
  
dV (x) ρ ρ 2
dx = − E(x)dx = − x dx or V (x) = − x + C2 .
dx s 2s
The boundary condition V (0) = 0 requires that C2 = 0 so the voltage in this planar detector is
ρ 2
V (x) = − x , (8.60)
2s
and the corresponding electric field is
dV ρx
E(x) = −
= . (8.61)
dx s
Notice that the voltage distribution is parabolic, while the electric field is linear.
The voltage normalized to unity at x = d is
 2& 2
V (x) ρx ρd x2
≡ Vn (x) = = 2, (8.62)
V (d) 2s 2s d
and is shown in Fig. 8.11. Also notice that the weight-
ing potential is linear, just as in a planar device with
no space charge while the operating potential is clearly
non-linear.
The above analysis for a planar device with uni-
form space charge reveals an important point: the space
charge in a detector does not affect the weighting poten-
tial distribution, but does affect the operating potential.
Intuitively, the result should be obvious because Gauss’
law shows that the electric field produced by a unit of
charge in a volume is independent of the electric fields
produced by other charges in the volume. Hence, the
induced current produced by the moving charge is in- Figure 8.11. A comparison of the weighting potential and
dependent of the electric field or potential produced by the normalized operating potential for a planar detector
the space charge, and produces the same effect as if with uniform space charge.
there were no space charge. The observed induced charge produced by a charge moving from one point to
another depends on the weighting potential between two specific points, and is independent of the trajectory
taken from one point in the detector to another.
However, the operating potential does affect the performance of the detector. The operating potential
and the accompanying electric field determine the charge carrier velocities and the active volume of a device.
The shape of the operating potential and the electric field also determines the charge carrier trajectories
as they travel through the detector volume. In gas-filled detectors, the operating potential determines
the operation region (ion chamber, proportional, Geiger-Müller). Further, for semiconductor devices the
operating potential determines the extent of recombination, trapping and detrapping effects.

7 The variation of the voltage and electric field in semiconductors is explored in greater detail in Chapter 15.
298 Essential Electrostatics Chap. 8

Historical Note
During the decade of the 1960s, there was some disagreement about the application of Ramo’s theorem to
detectors with space charge, or more precisely, about how the theorem could be applied to semiconductor
detectors. The confusion arose from the role of space charge in the depleted or active regions of the semicon-
ductor material, and how the charge induction from mobile free carriers was affected. As it turns out, space
charge within any radiation detector alters the electric field and, as a consequence, changes the charge car-
rier velocities. When analyzing a detector, one must take great caution in analyzing the operating potential,
which is found by solving Poisson’s equation for electric fields with the boundary condition that voltages
are set to the actual operating voltages. However, from Gauss’ law of electricity, the applied voltages do not
affect the voltage or electric field resulting from a point charge and, hence, the space charge also does not
affect the charge induction of a point charge as it moves in the cavity of the detector [Martini and Ottaviani
1969]. It can be concluded that (1) the analyst can use the normalized Laplace equation (weighting potential)
with all contacts grounded except for the collecting electrode to determine the charge or current induction
as a function of charge position and displacement, and (2) the analyst must use Poisson’s equation with the
actual operating voltages on all contacts to determine the charge carrier trajectories and velocities within
the detector cavity.

8.6.2 A Planar Detector Composed of Two Materials


In the previous analysis of a planar device, the medium between the two terminals was a single homogeneous
material. Now consider a planar device composed of two dielectric materials, as shown in Fig. 8.12. In such a
device, the electric field intensity is no longer constant in each material, although the dielectric displacement
is constant in each region.
x x The dielectric displacement is defined as
d1 1 d2 2

V+
D = s E, (8.63)

e1 e2 A where E is the electric field and s = κs o is the dielectric con-


stant of the material. Recall from Maxwell’s equations or, equiv-
alently, Gauss’ differential law of electricity that
x

0 d
∇•D = ∇•s E = ρ, (8.64)

where ρ is the space charge density. Note that Eq. (8.64) indi-
Figure 8.12. A planar detector composed of two
dielectric materials. cates that D must be constant if the space charge density is zero.
The dielectric constant is constant in most situations, so that Eq. (8.64) can represented as
ρ
∇•E = . (8.65)
s
However, in the device considered here, the dielectric constant is not constant across the device, and
Poisson’s equation cannot be used. Instead, for this one-dimensional geometry one has

d[s (x)E(x)] dE(x) ds (x)


= s + E(x) = ρ(x), (8.66)
dx dx dx
and if no space charge is present, as in the present case,

dE(x) ds (x)


s (x) + E(x) = 0. (8.67)
dx dx
Sec. 8.6. Charge Induction for a Planar Detector 299

For a detector with two different dielectric materials and no space charge in the device, the dielectric
displacement is constant and is given by
D =  1 E1 =  2 E2 .

However, the electric field across the device is not constant if the dielectric constants of both regions are not
the same. The voltage across the region between 0 to x1 , a width of d1 , is

V1 = (x1 − 0)E1 = d1 E1 ,

and across the region x1 to x2 , of width d2 , is

V2 = (x2 − x1 )E2 = d2 E2 ,

where the total voltage across the entire device is


 
d1 d2
VT = V1 + V2 = d1 E1 + d2 E2 = D + .
1 2

Here V1 and V2 are the voltage drops across region d1 and d2 , respectively. The capacitance of this detector
is
 
Q Q 1 2
C= = .
VT D d1 2 + d2 1

The voltage V (x) increases in a piecewise linear manner from V (0) = 0 to V (x2 ) = VT , i.e., as
⎧ xD

⎨ xE1 = , for x ∈ [0, x1 ]
1
V (x) = . (8.68)

⎩ (x − x2 )E2 + V1 = (x − x2 ) D + d1 D , for x ∈ [x1 , x2 ]
2 1

The weighting potential is thus Vw (x) = V (x)/VT .


If a gamma ray is absorbed in this planar device and produces No ion-electron pairs, the induced charge
after the ions and electrons have drifted and are separated by a distance Δx is



qNo D Δx qNo V1 Δx
⎨ VT 1 = VT d1 , 0 ≤ Δx ≤ x1

ΔQ = . (8.69)

⎪ qNo D Δx qNo V2 Δx

⎩ = , x1 ≤ Δx ≤ x2
VT 2 VT d2

Notice that charge induction increases as the dielectric constant decreases. Hence, a point charge moving
identical distances in both regions induces more charge when moving in the region of lower . One could
conceivably create a device that concentrates most of the charge induction to a small region with a low
dielectric constant, which is aligned with a larger volume with a high dielectric constant. In the present
case, the weighting potential and the operating potential for the device are identical in shape. The weighting
potential is scaled from 1 to 0, whereas the operating potential is scaled from the highest voltage Vhigh at
one contact to the lowest voltage Vlow at the opposite contact.
300 Essential Electrostatics Chap. 8

8.7 Charge Induction for a Cylindrical Detector


Often detectors are formed into cylindrical shapes, in which the active region is between an inner electrode of
radius r1 and an outer electrode of radius r2 . This geometry makes it possible to construct a volumetrically
large device while maintaining a relatively low capacitance on the smaller inner electrode. To take advantage
of the geometry and low capacitance, the signal is typically read from the smaller radius inner electrode.
The Laplacian operator for cylindrical geometry is
V+ A  
1 ∂ ∂V 1 ∂2V ∂2V
∇ V =
2
r + 2 + = 0. (8.70)
r ∂r ∂r r ∂φ2 ∂z 2
If the detector is a long coaxial cylinder, then the change in potential
with angle θ and length z is negligible, so that V (r, φ, z) → V (r)
r’2 and Eq. (8.70) reduces to
r0 g-ray
r’1  
1 d dV (r) dV (r) d2 V (r)
r1
∇ V =
2
r = +r = 0. (8.71)
-
++ - r2 r dr dr dr dr2
- ++-
+ -
Equation (8.71) can be rewritten as
electron-ion dE(r) d[E(r)r]
pairs E(r) + r =0 or = 0.
d dr
Because the derivative of E(r)r is zero, then the product must be a
Figure 8.13. Depiction of a cylindrical radi- constant, i.e., E(r)r = C1 or
ation detector where a gamma ray is absorbed
at radius r0 . The figure shows a preamplifier C1
attached to the positively biased inner elec- E(r) = . (8.72)
trode at r = r1 . r
The potential is then found as
 
C1
V (r) = E(r)dr = dr = C1 ln(r) + C2 . (8.73)
r
From Fig. 8.13, the preamplifier readout is seen to be attached to the inner electrode, which has a
positive bias V + . To find the potential, the inner electrode potential V (r1 ) is set to V + volts and the voltage
V (r2 ) on the outer electrode is set to zero. Use these
boundary conditions to evaluate the constants C1 and
C2 . Substitution for C1 and C2 in Eq. (8.73) gives
    −1
+ r r1
V (r) = V ln ln . (8.74)
r2 r2
The corresponding electric field, from Eq. (8.72), is
  −1
V+ r1
E(r) = ln . (8.75)
r r2
The weighting potential is found by setting V + = 1 in
Eq. (8.74), namely
    −1
Figure 8.14. Weighting potentials for various values of r r1
r1 /r2 versus the normalized distance from r1 to r2 for a Vw (r) = ln ln . (8.76)
cylindrical detector.
r2 r2
Sec. 8.8. Charge Induction for Spherical and Hemispherical Detectors 301

The weighting potentials, as a function of the ratio r1 /r2 for a cylindrical detector, are shown in Fig. 8.14.
At small values of r1 /r2 , the weighting potential shows a strong increase near the small anode, r1 . This
increase means that charges moving near the inner electrode create more induced charge than those free
carriers moving near the large outer electrode. Also it is seen that the weighting potential approaches that
of a planar detector as r1 /r2 approaches unity.
The ΔQ induced by the motion of free carriers as they drift toward the electrodes can be found from
Ramo’s theorem. After time t(r1 ) the electrons have drifted from where they were created at r0 to r1 and
after t(r2 ) the ions have drifted to a radial distance r2 . From Ramo’s theorem one has
 t(r2 )   t(r1 ) 
 
ΔQ = I(t) dt  + I(t) dt
0 ions+ 0 e−
 t(r2 )   t(r1 ) 
dr  dr 
= −qNo ∇Vw • dt − (−qNo ) ∇Vw • dt . (8.77)
0 dt ions+ 0 dt e−

In this geometry V is a function only of r so Eq. (8.77) is evaluated as follows.


 r2   r1 
dVw (r)  dVw (r) 
ΔQ = −qNo dr − (−q)No dr (8.78)
r0 dr ions+ r0 dr e−

Substitution of Eq. (8.76) for Vw (r) gives


  $    r1   /
−1 r2
r1 d r d r
ΔQ = −qNo ln ln dr − ln dr
r2 r0 dr r2 r0 dr r2
  −1 "      #
r2 r r
= qNo ln ln 2 − ln 1 (8.79)
r1 r0 r0
which yields the final result,
  −1  
r2 r2
ΔQ = qNo ln ln . (8.80)
r1 r1

This result shows that the induced charge is a function of only the total charge carrier displacement in r.
If the electrons drift to the positive contact at r1 and the positive ions drift to the negative contact at r2 ,
then r1 = r1 and r2 = r2 , and the induced charge becomes Q = qNo . It is important to note that the
weighting potential for a cylinder is not linear, and depends strongly upon the values of r1 and r2 , whereas
the weighting potential for the planar device is linear with x.

8.8 Charge Induction for Spherical and Hemispherical Detectors


Another detector configuration that has been successfully demonstrated is the hemispherical device, in which
a half sphere has the rounded outermost surface coated as the cathode contact and small spot at the center is
the anode contact. Typically, the preamplifier, used to measure the induced charge signal, is connected to the
small innermost contact. Fig. 8.15 shows a section of a spherical detector, which has the same characteristics
as a hemispherical detector. Ramo’s theorem is used to determine ΔQ induced by free charge carriers moving
in the device.
But first the weighting potential must be found. In spherical coordinates, the Laplacian for the detector
of Fig. 8.15 is
302 Essential Electrostatics Chap. 8

   
1 ∂ ∂V 1 ∂ ∂V 1 ∂2V
∇2 V = r2 + 2 sin θ + 2 2 = 0. (8.81)
r2 ∂r ∂r r sin θ ∂θ ∂θ r sin θ ∂φ2
Because of the spherical symmetry in the present geometry,
V+ A the potential changes with r but not with φ or θ. Equation (8.81)
then reduces to
 
1 d dV (r)
∇2 V = 2 r2 = 0, (8.82)
r’2 r dr dr
r0 g-ray
r’1 which can be rewritten as
 
r1 - r2 dV (r) r d2 V (r) d d[rV ]
++ - + = = 0.
- ++-
+ - dr 2 dr2 dr dr
Integration over r twice gives
electron-ion
pairs rV (r) = C1 r + C2 , (8.83)
where C1 and C2 are constants of integration to be found from
the boundary conditions. As before, the weighting potential is
Figure 8.15. Depiction of a spherical radia-
found from Eq. (8.83) with boundary conditions of Vw (r1 ) = 1
tion detector where a gamma ray is absorbed
at radius r0 . The figure shows a preamplifier and Vw (r2 ) = 0. The result is
attached to the positively biased inner elec-  
r1 r2
trode at r = r1 . Vw (r) = −1 . (8.84)
r2 − r1 r
The weighting potentials are shown in Fig. 8.16
as a function of the ratio r1 /r2 for a spherical (or
hemispherical) detector. At small values of r1 /r2 , the
weighting potential shows a strong increase near the
small anode at r1 , which means that charges moving in
the vicinity near the inner contact have more influence
on the induced charge than those free carriers moving
near the large electrode at r2 . As with the cylindri-
cal detector, the weighting potential approaches that
of the planar device as r1 /r2 approaches unity. One
should notice that the weighting potential for a spher-
ical detector is much more skewed than for the cylin-
drical detector.
Figure 8.16. Weighting potentials for various values of The induced charge is now found with Ramo’s The-
r1 /r2 versus the normalized distance from r1 to r2 for a orem with the contributions of the electrons and ions
spherical detector. being analyzed separately. Because Vw (r) is a function
of only r, as in the previous cylindrical geometry, Eq. (8.78) is applicable to the spherical geometry as well.
Substitution of the weighting potential from Eq. (8.84) into Eq. (8.78) yields
  $ r2  r2 /
r1 d r2 d r2
ΔQ = −qNo dr − dr
r2 − r1 r0 dr r r0 dr r
  "   #
r1 r2 r2 r2 r2
= qNo − − − ,
r1 − r2 r2 r0 r1 r0
Sec. 8.9. Concluding Remarks 303

which, upon rearrangement, yields the final result,

r1 r2 r1 − r2
ΔQ = qNo . (8.85)
r1 r2 r1 − r2

8.9 Concluding Remarks


The topics discussed in this chapter constitute the fundamental physics governing radiation detectors whose
signal formation is based on current induction. The reader is referred to the references for sources with more
detailed discussions on electricity and magnetism. It should be noted there are circumstances, not covered
in the present chapter, that can alter detector performance. For instance, current induction in gas-filled ion
chambers may depend mainly upon the motion of electrons, and in other gas-filled detectors the current
induction may depend mainly on positive ion motion. Semiconductor detectors, based on current induction,
may have imperfections that cause an exponential decrease of the charge carrier density with time, thereby
causing the current induction to be a function of time, charge carrier velocity, and interaction position. Such
alterations in detector response are described in the chapters on gas-filled and semiconductor detectors.
Further, unique detector electrode designs can be used to change the current induction contributions of
electrons and positive ions as a function of position, as shown here for the cylindrical and spherical devices.
In the absence of space charge, the weighting and operating potentials of two-terminal devices have essentially
the same shape, the difference being the former is normalized and the latter is not. In the presence of space
charge, the shapes of the weighting and operating potentials can be significantly different.

PROBLEMS
1. A charge of 2.5 × 10−8 C is placed in an upwardly directed electric field with magnitude 5 × 104 N C−1 .
Determine the work performed for the following three cases: (a) the charge is moved 24 cm to the right,
(b) the charge is moved 24 cm downward, and (c) the charge is moved 34 cm at a downward 45◦ angle.
2. A 5.5 MeV alpha particle has a direct head-on collision with a Au nucleus at rest. What is the minimum
distance achieved between the two particles?
3. There are two point charges placed 1 cm apart, where
Q1 = +qe N1 = qe (104 ) and Q2 = −qe N2 = −qe (5 × 103 ).
Determine: (a) the potential halfway between the two charges, (b) the potential at a point exactly 6
mm from Q1 and 8 mm from Q2 , and (c) the work performed moving the charge from the location of
B to the location of A.
4. Consider an evacuated parallel plate chamber with 1000 volts applied between the contacts spaced 3 cm
apart. Simultaneously, an electron is released from the cathode and a He 2+ ion is released from the
anode. (a) At what distance from the positive electrode do the particles pass each other? (b) What are
the particle speeds when they arrive at their respective collection electrodes? (c) What are the particle
energies when they arrive at their respective collection electrodes?
5. For a cylindrical capacitor with dielectric constant s , inner conductor radius ra and outer conductor
radius rb , (a) derive an expression for the capacitance per unit length. (b) Derive an expression for the
total capacitance of a hemispherical capacitor.
304 Essential Electrostatics Chap. 8

6. Consider the diagram below (Fig. 8.17). An electron is released from electrode C and travels through
electrode B to electrode A at constant speed. (a) Sketch the output pulse from the electron if measured
from electrode A. (b) Sketch the output pulse from the electron if measured from electrode C. (c) Sketch
the output pulse from the electron if measured from electrode B.

e-

A B C

Figure 8.17. Diagram for problem 6.

7. You have a coaxial detector filled with 1 atm Ar and with inner electrode radius of 25 microns and outer
electrode radius of 1.25 cm. A potential of 1000 volts is applied. A radiation interaction occurs at radius
r = 0.625 cm, producing 50,000 electron-ion pairs. Sketch the pulse shape as a function of time for: (a)
positive voltage applied to the inner electrode and (b) negative voltage applied to the inner electrode.

REFERENCES
BECK, A.H.W., Thermionic Valves, London: Cambridge Univer- Semiconductor Detectors,” Nucl. Instrum. Meth., 67, 177–178,
sity Press, 1953. (1969).
JACKSON, J.D., Classical Electrodynamics, 2nd Ed., New York: RAMO, S., “Currents Induced by Electron Motion,” Proc. IRE,
Wiley, 1975. 27, 584–585, (1939).
RILEY K.F., M.P. HOBSON, AND S.J. BENCE, Mathematical Meth-
JEANS, J., The Mathematical Theory of Electricity and Mag-
ods for Physics and Engineering, 3rd Ed., Cambridge: Cam-
netism, 5th Ed., London: Cambridge University Press, 1943.
bridge University Press, 2006.
JEN, C.K., “On the Induced Current and Energy Balance in Elec- SHOCKLEY, W., “Currents to Conductors Induced by a Moving
tronics,” Proc. IRE, 29, 345–349, (1941). Point Charge,” J. Appl. Phys., 9, 635–636, (1938).
MARTINI, M. AND G. OTTAVIANI, “Ramo’s Theorem and the En- SMYTHE, W.R., Static and Dynamic Electricity, 3rd Ed., Bristol:
ergy Balance Equations in Evaluating the Current Pulse from Taylor & Francis, 1989.
Chapter 9

Gas-Filled Detectors:
Ion Chambers
Gases are distinguished from other forms of matter, not only by their power of indefinite
expansion so as to fill any vessel, however large, and by the great effect heat has in dilating
them, but by the uniformity and simplicity of the laws which regulate these changes.
James Clerk Maxwell

In 1908, Ernest Rutherford and Hans Geiger constructed the first gas-filled radiation detector from a metallic
cylinder with a thin axially positioned wire inside [Rutherford and Geiger 1908]. The gas medium in this
case was air. When a voltage was applied between the cylinder and wire, a current was measured with an
electrometer when alpha particles entered the device. They also noticed that the behavior of the detector
changed with increasing voltage, namely, that alpha particles could be detected at much lower applied
voltages than beta particles. This ability to discriminate between the two radiations became known as
proportional counting. Experiments conducted later with the gas-filled detectors clearly showed distinctive
regions of operation, as shown in Fig. 9.1.
The physical principle behind a gas-filled detector is quite simple. Radiation interacts in either the
chamber gas or the chamber walls, thereby liberating electrons from parent nuclei. These electrons (and
ions in the gas) produce additional ionization in the detector gas, which creates a charge “cloud” composed
of electrons and positive ions. A voltage placed across electrodes in the gas chamber causes the electrons
and ions to drift apart in opposite directions, with electrons drifting towards the anode and the positive ions
drifting towards the cathode. In some cases, electron attachment to a neutral atom produces negative ions.
As these gas ions and electrons, or charge carriers, move through the chamber, they induce a current to flow
in an external circuit connected to the chamber. This current, or change in current, can then be measured
as an indication that a radiation interaction occurred in the chamber.

9.1 General Operation


Gas detectors can be operated in either a pulse mode or current mode. Pulse mode is generally used in
low to moderate radiation fields. In this case, a single radiation particle, such as an alpha particle, beta
particle, or gamma ray, interacts in the chamber volume, producing a charge cloud around the interaction
site. The charge carriers then drift apart and induce current between the device terminals. A charging
circuit, usually consisting of a preamplifier and feedback circuit, time-integrates the current and records a
voltage pulse. This voltage pulse is treated as a single event, i.e, a single radiation particle has been detected.
The preamplifier circuit is subsequently discharged and reset, so as to allow the device to detect the next
radiation-interaction event. Hence, each voltage pulse from the detector indicates a radiation interaction
event. Although extremely useful, there are drawbacks to pulse-mode operation. Should another radiation
interaction occur while the detector is integrating or discharging the current from a previous interaction

305
306 Gas-Filled Detectors: Ion Chambers Chap. 9

ion pair recombination event, the detector may not, and usually does
occurs before collection
not, record the new interaction, a condition
Geiger-Muller
onset of region
“gas multiplication” referred to as pulse pile up. The time interval
in which a new pulse is not recorded is the de-
transition
Pulse Height or Ions Collected

region tector recovery time, also referred to as dead


time (see Ch. 7). A pulse-mode detector oper-
ated in low radiation fields has little problem
(log scale)

I II III with dead time; however, a detector operated


in high radiation fields may have significant
dead time losses, thereby yielding an incorrect
a particles measurement of the radiation intensity.
For high radiation fields, gas detectors are
commonly operated in current mode, in which
IIIa IV V the radiation induced current is measured with
a current meter. Under such conditions, many
b particles interactions can occur in the device in very
short periods of time, and the current observed
Detector High Voltage (volts) increases with radiation exposure. Hence, cur-
rent mode can be used to measure high ra-
Figure 9.1. The observed output pulse height versus the applied
high voltage for a gas-filled detector. Several different regions can be
diation fields in which the magnitude of the
seen: (I) recombination, (II) ion chamber, (III) proportional, (IIIa) current is a measure of the radiation induced
transition region, (IV) Geiger-Müller, and (V) continuous discharge. ionization rate in the detector. The output
current is then proportional to the intensity
of the radiation field at the detector location. The drawback to pulse-mode operation is that it does not
distinguish between individual radiation interactions.
Consider a gas-filled detector as shown in
Electron-Ion CUT AWAY VIEW Fig. 9.2, similar to the device first devised by
Pairs
Thin Window
Geiger and Rutherford, in which α-particles
Insulator
+- and β-particles enter through a thin window.
-+ + - These particles can interact in the gas (or tube
+- - -
+ + wall) depositing some or all of their energy in
the tube gas and, in the process, generate a
Ionizing miniature cloud of free electrons and positive
Radiation
ions, referred to as electron-ion pairs. As re-
quired for any radiation detector, there is an
Anode Wire absorber (the fill gas), and an observable (the
Gas Container electron-ion pairs). To complete the detector,
and Cathode
a method is needed to measure the amount
Figure 9.2. Shown is a coaxial gas detector, which is commonly of ionization. Suppose the detector is con-
used for Geiger-Müller tubes, and sometimes used for proportional nected to a simple electrometer so as to mea-
counters. High voltage is applied to the central wire anode, while the
outer cylinder wall, the cathode, is held at ground.
sure the current produced by the motion of the
electron-ion pairs. Without an applied volt-
age, the electron-ion pairs diffuse randomly in all directions and eventually recombine. As a result, the net
current measured by the electrometer is zero. However, if a small positive voltage is applied to the central
thin wire (anode) of the device, the free electrons (negative charges) drift towards the anode and the free ions
(positive charges) drift towards the detector wall. At low voltages, some measurable current is observed, yet
considerable recombination will still occur, the expected result within Region I, the recombination region, as
Sec. 9.2. Electrons and Ions in Gas 307

shown in Fig. 9.1. As the voltage is increased, electron-ion pair separation is more rapid until practically no
recombination occurs. Hence, the current measured is a measure of the total number of electron-ion pairs
formed. This is Region II, and is referred to as the ionization chamber region.
As the voltage is increased further, the electrons gain enough kinetic energy from the electric field to
create more electron-ion pairs through impact ionization, thereby providing a mechanism for signal gain,
often referred to as gas multiplication. As a result, the observed current increases as the voltage increases,
but the amount of ionization is still proportional to the energy deposited in the gas by the original radiation
particle. This is Region III, the proportional region. Still further increasing the applied voltage causes
disproportional current increases to form, labeled in Fig. 9.1 as the transition region IIIa, beyond which, in
Region IV, all currents, regardless of origin, radiation species or energies, have the same magnitude. Region
IV is the Geiger-Müller region. Finally excessive voltage drives the detector into region V where the voltage
causes sporadic arcing and other spontaneous electron emissions to occur, causing continuous discharging in
the detector. Because of possible equipment damage and the loss of meaningful signals, gas detectors should
not be operated in the continuous discharge region. In the following chapter, detector operation in Regions
I and II is described.

9.2 Electrons and Ions in Gas


Radiation interactions in gas can cause excitation and ionization. Excitation is a process in which the energy
transferred to a gas atom or molecule is less than the ionization energy. Hence, electrons are elevated to a
higher energy level, but are still bound to the nucleus. Energy transferred to electrons greater than their
ionization energy causes ionization, so that the electrons and positive ions become separate charge carriers.
An electric field applied to the gas volume separates these charge carriers and, in the process, produces an
induced current, as described in Chapter 8. The electrons, with a mass more than a thousand times less than
that of the positive ions, also have quite different transport properties than heavy ions. Also, negative ions,
formed from electron attachment to neutral atoms, have different transport characteristics than positive ions
(although similar). Detector and gas properties that affect the charge transport for electrons and ions include
mobility, electric field, ionization potential, charge transfer, electron attachment, and recombination. In the
following chapter on gas-filled ion chambers, pertinent information on charge transport and ion behavior
in gases is presented. Exhaustive studies dedicated to the complexities of electron and ion motion in gases
have been published in far more detail than presented here. See, for example, [Loeb 1939, 1960; Huxley and
Crompton 1974; Sitar et al. 1993].

9.2.1 Ionization
Directly ionizing radiation with energy above the minimum ionizing energy I0 of a gas will produce electron-
ion pairs (eip) along their trajectories. Due to competing energy loss mechanisms, such as atomic excitation
and bremsstrahlung production, the average energy w required to produce an electron-ion pair is typically
much greater than I0 . As the ionizing particle passes through the detector gas, it produces a continuous
chain of electron-ion pairs. The total number of electron-ion pairs produced per unit distance of travel by
the charged particle is
dE 1
nt  . (9.1)
dx w

Note that, although Eq. (9.1) may be used to estimate the density of ion pairs per unit path length, the
stopping power dE/dx for heavy ions (alpha particles, for instance) is not constant. The values for nt and
dE/dx in Table 9.1 are listed for minimum ionizing particles (MIPs), i.e., beta particles with energies above
308 Gas-Filled Detectors: Ion Chambers Chap. 9

Table 9.1. Useful properties of various gases at 293 K and 760 torr. From [Sauli 1977].

ρo (1 atm) Io w (dE/dx)/ρo dE/dx np nt


Gas Z A
g/cm3 eV eV/eip* MeV g−1 cm2 keV/cm eip*/cm eip*/cm

H2 2 2 8.38 × 10−5 15.4 37 4.03 0.34 5.2 9.2


He 2 4 1.66 × 10−4 24.6 41 1.94 0.32 5.9 7.8
N2 14 28 1.17 × 10−3 15.5 35 1.68 1.96 (10) 56
O2 16 32 1.33 × 10−3 12.2 31 1.69 2.26 22 73
Ne 10 20.2 8.39 × 10−4 21.6 36 1.68 1.41 12 39
Ar 18 39.9 1.66 × 10−3 15.8 26 1.47 2.44 29.4 94
Kr 36 83.8 3.49 × 10−3 14.0 24 1.32 4.60 (22) 192
Xe 54 131.3 5.49 × 10−3 12.1 22 1.23 6.76 44 307
CO2 22 44 1.86 × 10−3 13.7 33 1.62 3.01 (34) 91
CH4 10 16 6.70 × 10−4 13.1 28 2.21 1.48 16 53
C4 H10 34 58 2.42 × 10−3 10.8 23 1.86 4.50 (46) 195

* eip = electron-ion pair

1 MeV.1 The total number NT of electron-ion pairs produced by a beta particle can then be estimated with
the measured data listed in Table 9.1 as
ΔE
NT  , (9.2)
w
where ΔE is the energy deposited in the gas. The initial ionizing particle creates np primary electron-ion
pairs per unit length as it passes through the detector gas and deposits ΔE of energy. If ΔE I0 , the
energetic free electrons and positive ions can have sufficient kinetic energy to produce more electron-ion
pairs through secondary ionization (delta rays). By summing contributions from primary and secondary
ionization, the total density of electron-ion pairs per unit pathlength, nt , can be found. Values of np and
nt for several common detector gases are listed in Table 9.1. For mixtures of different gases, a general rule
often used to describe the total number of ion pairs created is


K
fi ΔE
NT  , (9.3)
i=1
wi

where fi is the concentration fraction of each gas constituent. The total ionization, per unit path length of
travel, for MIPs is
K
ρ
nt  fi nit , (9.4)
i=1
ρ◦

where ρ◦ is the gas density at 1 atm, ρ is the gas density at the operating pressure, and nit is nt for gas
species i. Similarly, the primary ionization per unit path length for MIPs is


K
ρ
np  fi nip . (9.5)
i=1
ρ◦

1 From Fig. 4.20 the collisional stopping power for electrons is nearly constant for energies above about 1 MeV.
Sec. 9.2. Electrons and Ions in Gas 309

9.2.2 Diffusion Effects


Following the creation of the electron-ion pairs, the ions and electrons begin to diffuse to regions with lower
charge densities according to Fick’s law of diffusion. Also the initial high concentration of electrons and
positive ions promotes recombination losses. Because the electron mass is much less than that of a positive
ion, the electrons diffuse much faster than the positive ions. This phenomenon has a significant effect on
detector operation and performance.
Diffusion of Electrons in a Gas
After the initial ionization event, the electrons and ions rapidly come into thermal equilibrium with the gas
and assume a Maxwellian distribution of speeds ωe and ωion . The number density for the electron thermal
speed ωe distribution in a charge cloud is given by
 
me 3/2 2 me ωe2
ne (ωe ) = 4π ωe exp − , (9.6)
2πkT 2kT
where me is the electron mass. The average electron thermal speed ω e is
 ∞ & ∞ 
8kT
ωe = ωe n(ωe ) dωe n(ωe ) dωe = . (9.7)
0 0 m eπ

In terms of energy, the number density for the electron energy distribution in a charge cloud is
 3/2  
1 √ E
ne (E) = 2π E exp − , (9.8)
πkT kT
and the average electron energy is2
 ∞ & ∞
3kT
Ee = E n(E) dE n(E)dE = . (9.9)
0 0 2
The diffusion rate of the electrons and ions, to a first approximation, can be evaluated with Fick’s law,
namely,
dne (r, t)
= De ∇2 ne (r, t), for electrons, (9.10)
dt
dnion (r, t)
= Dion ∇2 nion (r, t), for ions. (9.11)
dt
Here De and Dion are the diffusion coefficients for electrons and ions with units of cm2 /s, and ne (r, t) and
nion (r, t) are the charge carrier concentrations. Also, r is the distance from the center of the initial charge
cloud whose size is negligible compared to volume of the gas tube. Thus, all charges are assumed to begin
to diffuse radially outwards from r = 0. In this spherically symmetric coordinate system Eq. (9.10) can be
written as    
∂ne (r, t) 1 ∂ ∂ne (r, t) 2 ∂ne (r, t) ∂ 2 ne (r, t)
= De 2 r2 = De + . (9.12)
∂t r ∂r ∂r r ∂r ∂r2
The solution for ne (r, t) in three dimensions in an infinite gas medium is
 
n0 −r2
ne (r, t) = exp , (9.13)
(4πDe t)3/2 4De t

2 Note 1
that m ω2
2 e e
= Ee.
310 Gas-Filled Detectors: Ion Chambers Chap. 9

where n0 is the initial number of electrons. The


  mean distance squared r2 is
  ∞ & ∞
 r2 = ne (r, t) r2 dV ne dV = 6De t.
   


 0 0
 (9.14)

Often a simpler one-dimensional diffusion
 model is used in which electrons diffuse away from
a plane of electrons created at t = 0 containing n0

electrons cm−2 . Then in Eq. (9.10) ∇2 → d2 /dx2
  where x is the perpendicular distance from the
plane source. The solution in an infinite homo-
 geneous gas medium is
    
       
n0 −x2
ne (x, t) = √ exp , (9.15)
Figure 9.3. Diffusion of an electron cloud based upon 4πDe t 4De t
Eq. (9.15).
which is recognized as a normal (Gaussian) distribution function with mean x = 0 and variance 2De t. The
diffusion of electrons as a function of time in a gas, according to Eq. (9.15), is illustrated in Fig. 9.3.
The Diffusion Coefficient De
The momentum-transfer cross section for electrons is defined as [Buckman and Elford 2000]
 π  
dσ v
σm (E) = 2π 1− cos θ sin θ dθ, (9.16)
0 dΩ v0

where dσ/dΩ is the differential scattering cross section, v0 is the initial electron speed, and v is the electron
speed after scattering. The momentum-transfer cross sections for several gases used in radiation detectors
are shown in Fig. 9.4. There is a notable decrease in the cross section for Ar, Kr, and Xe gases between
the energies of 0.1 eV to 1 eV, known as the Ramsauer-Townsend effect, a consequence of the quantum
mechanical wave nature of low-energy electrons and their resonant transmission through the potentials of
select gases. The differential scattering cross section is defined as the fraction of electrons of energy E that
scatter at angle θ into differential solid angle dΩ, where dΩ = 2π sin θdθ. The electron diffusion coefficient is
given by [Rice-Evans 1974]
ωe
De = , (9.17)
3na σm
where na is the molecular density at temperature T (absolute) and pressure P (torr) and is found from

P T0
na = nL . (9.18)
P0 T

Here nL is the Loschmidt constant,3 defined as

P0 P0 NA
nL = = , (9.19)
kT0 RT0

3 The Loschmidt constant is the atomic or molecular density for an ideal gas, quoted as 2.6867774 × 1019 cm−3 at 0◦ C at 760
torr.
Sec. 9.2. Electrons and Ions in Gas 311


  













 


Figure 9.4. The measured momentum transfer cross section of electrons in various
gases. From [Phelps 1985; Buckman and Elford 2000; Itikawa 2006].

where P0 = 760 torr, T0 = 273K, NA is Avogadro’s number, R is the gas constant,4 and k is Boltzmann’s
constant. The frequency between collisions is [Sitar et al. 1993]

νe = na ωe σe = τe−1 , (9.20)

where σe is the elastic scattering cross section for electrons, ωe is the average electron thermal speed and τe
is the average collision time. Note that σe = σm for isotropic scattering; hence, the mean free path between
collisions is
1 kT
λe = = . (9.21)
na σm P σm
Substitution of Eq. (9.7) and Eq. (9.21) into Eq. (9.17), the diffusion coefficient for the average electron
energy is
ω e λe (2kT )3/2 1
De = = √ . (9.22)
3 me π 3P σm
The diffusion of electrons in a gaseous medium is largely governed by the concentration gradient and the
diffusion coefficient. However, Coulombic attraction and repulsion between ions and electrons can alter the
motion of electrons in the gas from the ideal diffusion model for neutral particles.

4R = 8.3144621 molJ K
.
312 Gas-Filled Detectors: Ion Chambers Chap. 9

Different mixtures and concentrations of gases can be used to alter the diffusion properties. For instance,
adding gases that have low σm values increases De and, consequently, increases the electron diffusion. Like-
wise, diffusion can be hindered by adding gases that have large σm values. An estimate of the diffusion
coefficient can be found with [Sitar et al. 1993] as
 −1
 Pi
De = , (9.23)
i=1
Di

where Pi is the relative partial pressure of each gas and Di is the diffusion coefficient of each gas.
Diffusion of Ions in a Gas
The equations developed for electron diffusion in a gas hold true for ion diffusion. Hence, the one-dimensional
solution of Eq. (9.15) gives
 
n0 −x2
nion (x, t) = √ exp , (9.24)
4πDion t 4Dion t
where the mean squared distance r2 = 2Dion t, which is also the variance of the normal distribution of
Eq. (9.24). The diffusion coefficient is

ω ion λion (2kT )3/2 1


Dion = = √ , (9.25)
3 mion π 3P σion

where λion , ωion , and mion are the ion counterparts of λe , ω e and me , respectively. Note that the diffusion
coefficient is inversely proportional to the square root of the ion mass. For this reason the diffusion coefficients
for ions are significantly smaller than that for electrons, as can be seen from Table 9.2. Consequently, the
diffusion speed of ions can be over 1000 times less than that of electrons.

9.2.3 Electron and Ion Transport


As explained in Chapter 8, it is the motion of charges in some preferred direction that induces current flow
in an electronically operated detector. However, if both negative and positive charges are moving equally
in all directions, as occurs in the diffusion of both electrons and ions, then the net induction current must
be zero. Although there is no induced current, the diffusion process still causes the electrons and ions to
separate because the ions diffuse much more slowly than do the electrons.
But with the application of an electric field to the chamber, the electrons and ions further separate and
begin to drift in opposite directions. This motion in a preferred direction then induces a current, whose
measurement indicates that an ionizing event has occurred in the detector.
Influence of an Electric Field
The average kinetic energy of thermal electrons in a gas at 20◦ C is given by the Boltzmann distribution

3kT
Ee = = 0.038eV. (9.26)
2
This average energy corresponds to a speed of ωe = 4.2 × 107 cm/s. Yet, these randomly oriented trajectories
produce no induced current in the detector.
The application of an electric field E exerts a force on the diffusing electrons and ions causing the electrons
to drift preferentially towards the anode and the ions to drift preferentially towards the cathode. However,
the drift speeds are typically very much less than the thermal motion speeds. For electrons the drift speeds
Sec. 9.2. Electrons and Ions in Gas 313

Figure 9.5. The characteristic energy as a function of electric field for Ar gas at 1
ATM. After [Palladino and Sadoulet 1975].

are on the order of 105 to 106 cm/s. The average electron drift speed ve of the electrons in the direction of
the applied electric field is approximated by Palladino and Sadoulet [1975] as

qe E λe
ve = , (9.27)
me ω e

where qe is the unit electronic charge. A measurable quantity, referred to as the electronic characteristic
energy, K , is a function of the diffusion coefficient and the electric field, namely, [Rice-Evans 1974]

qe D e E qe D e
K = = . (9.28)
ve μe

and De is given by Eq. (9.22). The electronic characteristic energy is the effective kinetic energy of the free
electron in an electric field. It is much greater than that for electrons undergoing only thermal diffusion.
Measured and calculated values of K for pure Ar are shown in Fig. 9.5. Theoretical and measured values of
K as a function of reduced electric field (E/P ) for many gases can be found in the literature [Christophorou
1971; Schultz and Gresser 1978; Peisert and Sauli 1984]. The quantity

qe λe
μe = , (9.29)
me ω e

is commonly referred to as the electron charge carrier mobility.5

5 Loeb [1960] reviews alternative, but similar, expressions for electron mobility.
314 Gas-Filled Detectors: Ion Chambers Chap. 9

From Eq. (9.27) and Eq. (9.29), the drift speed in the presence of an electric field is thus given by the
simple relation
ve = μe E, (9.30)
in which the charge carrier mobility is a function of gas pressure, namely,
P0 μ0
μe = , (9.31)
P
where μ0 is the mobility in units of cm2 V−1 s−1 at 1 atm (760 torr) pressure, P0 = 760 torr, E is the electric
field, and P is the gas pressure in torr.
The mobility is related to the diffusion coefficient by6
De kT
= (9.32)
μe qe
where De is the electron diffusion coefficient, qe is the unit charge of an electron, k is Boltzmann’s constant
and T is the absolute temperature. Equation (9.30) is valid up to a saturation electric field Esat , beyond
which charged particle scattering becomes the determining factor for the drift speed. At low fields, the
electron drift speed is linear with respect to the applied field; however, this region of linearity is usually
below a reduced electric field value of 0.3 V cm−1 torr−1 for many important detector gases. As electrons
gain energy under higher electric fields, their small mass allows high speeds to be reached with moderately
low voltages. Electron collisions with other electrons in the gas can cause more ionization, referred to as
impact ionization, which increases the number of electron-ion pairs in the gas, but such collisions reduce
the mean free path of the electrons. As a result, electrons reach a saturation speed vsat at electric fields
approaching Esat .
Consider the ratio ξ between the characteristic energy (for any value De and associated μe ) and the
average thermal energy, namely
K 2qe De
ξ= = . (9.33)
Ee 3μe kT
Substitution of Eq. (9.32) into Eq. (9.33) and rearrangement gives

De 3kT
=ξ . (9.34)
μe 2qe
The electron drift speed, for the same reduced electric field, varies among detector gases and gas mixtures.
In argon, a common detector gas, electrons reach a fairly constant saturation speed of approximately 0.37
cm μs−1 at a reduced electric field of 0.2 V cm−1 torr−1 , as can be seen from Fig. 9.6. However, the small
addition of 0.2% nitrogen increases the saturation speed above 1.0 cm μs−1 (at 0.6 V cm−1 torr−1 ). From
the data shown in Fig. 9.6, the mean drift speed for electrons in pure argon gas can be approximated by

3.64(E/P ) + 114.6(E/P )2
ve = cm/μs, (9.35)
1 + 12.7(E/P ) + 304.33(E/P )2

6 Eq. (9.32) is commonly called the Einstein relation because it appeared in his 1905 paper in Annalen der Physik. On rare
occasion, Eq. (9.32) has been called the Einstein-Smoluchowski relation because it was published later by Smoluchowski [1906]
(also in Annalen der Physik with reference to Einstein’s 1905 paper). However, as pointed out by Huxley [1974], Nernst [1888]
published the relation for electrolytic ions in 1888. Townsend [1900] applied a form of Eq. (9.32) to gases and published it in
1900 in Philosophical Transactions A, although in a considerably less recognizable form. Regardless, it has been suggested by
Huxley [1974] that the proper name for Eq. (9.32) should be the Nernst-Townsend relation due to their prior publications.
Sec. 9.2. Electrons and Ions in Gas 315

Figure 9.6. The measured drift speed of electrons in argon/nitrogen mixtures as a


function of reduced electric field (E/P) and nitrogen concentration;  pure argon;
0.05% N2 ;  0.1% N2 ; ◦ 0.2% N2 . After [Bortner et al. 1957].

Figure 9.7. The measured drift speed of electrons in P-10 gas (90% argon, 10%
methane) as a function of reduced electric field (E/P ). Data from  [Bortner et al.
1957]; ◦ [Mattern 1988];  [Ferreira et al. 2005]. Discrepancies between measured
values may be due to impurity contamination in the gas samples.
316 Gas-Filled Detectors: Ion Chambers Chap. 9

Figure 9.8. The measured drift speed of electrons in various organic polyatomic
gases as a function of reduced electric field (E/P ); • CH4 ;  C2 H6 ; C2 H 4 ;
 C3 H8 ; and 2 C2 H2 . After [Cottrell and Walker 1965].

where E/P ≤ 0.8 V cm−1 torr−1 .


Another common detector gas is a mixture of 90% Ar and 10% CH4 , generally referred to as P-10 gas.
Electrons reach a maximum speed at reduced electric fields between 0.2 and 0.3 V cm−1 torr−1 , beyond
which electron scattering causes the speed to drastically decrease as can be seen in Fig. 9.7. With the data
of Fig. 9.7, the mean drift speed for electrons in P-10 gas can be approximated by

6.852 E/P + 4.626(E/P )
ve =  cm/μs, (9.36)
1 − 3.306 E/P + 6.059(E/P )
where E/P ≤ 1.4 V cm−1 torr−1 .
Drift speeds of many other organic gases used in
gas-filled detectors are shown in Fig. 9.8. Note that
CH4 has a similar electron drift speed characteristic as
P-10 gas, with a maximum of approximately 10.5 cm
μs−1 , whereas the other organic gases shown in Fig. 9.8
do not show this trend, but instead gradually approach
a saturation speed.
The drift speed of ions, having much smaller mo-
bilities than electrons because of their much larger
masses, typically follow Eq. (9.30) for electric fields
commonly used in ion chambers (or other gas-filled
detectors). Measured ion mobilities (μ0 ) for several
gases, as reported by different sources, are listed in
Table 9.2.
The motion of charge carriers within an electric Figure 9.9. Diffusion and drift of an electron cloud based
upon Eq. (9.37).
field is influenced by the combined effects of diffusion
Sec. 9.2. Electrons and Ions in Gas 317

Table 9.2. Transport properties of various ions in the same gas at 1 atm. Data are from [Loeb
1929; Rossi and Staub 1949; Staub 1953; Sharpe, 1964; Huxley 1974; and Sauli 1977].
+
λion ω ion Dion μ+
ion

Dion μ−
ion
Gas
cm cm s−1 cm2 s−1 cm2 V−1 s−1 cm2 s−1 cm2 V−1 s−1

Air 0.028 1.36 0.043 1.87


Ar 1.0 × 10−5 4.4 × 105 0.04 1.7 0.043 1.7
H2 1.8 × 10−5 2 × 105 0.123 6.7 .190 7.95
C2 H 2 0.018 0.71 0.021 0.86
C2 H 4 .019 0.75
C2 H 6 0.027 1.07
Cl2 0.018 0.73
CO 0.027 1.1 0.027 1.07
CO2 6 × 10−6 5.5 × 105 0.023 0.76 0.026 0.81
H2 O 1.0 × 10−5 7.1 × 105 0.02 0.7 0.019 0.75
He 2.8 × 10−5 1.4 × 105 0.26 10.2 0.157 6.31
Ne 4.4
N2 3 × 10−5 9.0 × 105 0.032 1.27 0.045 1.82
O2 1.0 × 10−5 5.0 × 105 0.025 1.36 0.0396 1.80

and drift. The distribution of electrons or ions as a function of electric field and time is
 
n0 −(x − μi Et)2
ni (x, t, E) = exp , (9.37)
(4πDi t)1/2 4Di t
where the subscript i refers to electrons or ions, v i = μi E ≤ vsat . The diffusion and drift of electrons in a
gas as a function of time, according to Eq. (9.37), is illustrated in Fig. 9.9.

9.2.4 Charge Transfer


Heavy positive ions colliding with neutral molecules (or atoms) can exchange charge, i.e., a singly charged
positive gas ion accepts an electron from a neutral gas component, thereby becoming neutralized while
ionizing the previously neutral molecule. For ions moving in the same host gas, for instance Ar+ moving
through Ar, an electron can be transferred from a neutral gas atom to a positively charged gas ion, referred
to as symmetric resonance charge transfer [Sitar et al. 1993],
X + + X → X + X +, (9.38)
−15 −14 2
with a cross section on the order of 10 to 10 cm . This form of charge transfer effectively reduces the
mobility of positive ions in the same neutral gas, quoted as being on the order of 7.5% reduction in mobility
from that of the neutral gas atom [Wilkinson 1950].
In many cases, a second gas is purposely introduced in with the main detector gas to alter the ion
transport characteristics. The ability for a positive ion to pick up an electron in a collision is strongly
dependent upon the separate ionization potentials. If the ionization potential of the host gas is higher than
that of the added neutral gas atoms or molecules, then charge transfer from host gas ions colliding with
neutral gas molecules (atoms) of the second component is possible, whereas the reverse electron exchange
is not. This type of charge transfer is referred to as asymmetric non-resonance charge transfer [Sitar et al.
1993] and is written as
X + + Y → X + Y + + Δ, (9.39)
where Δ is the difference in ionization energies (I0X − I0Y ), and has a charge transfer cross section of about
10−15 cm2 . For instance, the introduction of CH4 (I0 = 13.1 eV) into Ar (I0 = 15.8 eV) permits charge
318 Gas-Filled Detectors: Ion Chambers Chap. 9

transfer to occur between Ar+ and CH4 , but not the reverse exchange. Hence,

Ar+ + CH4 → Ar + CH+


4 + 2.7 eV. (9.40)

In the next chapter on proportional counters, this reaction is seen to be a very important charge transfer
reaction. If the detector gas is a mixture of both Ar and CH4 , ionizing radiation creates a cloud of both
Ar+ and CH+ 4 ions. However, within a short period of time, ion exchange causes virtually all Ar atoms to
become neutralized, having transferred their charge to the CH4 molecules.

9.2.5 Electron Attachment


After the initial charge cloud has been formed, the electric field separates the positive ions and electrons.
Electrons, having significantly higher mobility than ions, rapidly drift towards the detector anode, while the
positive ions slowly drift towards the cathode. There is a possibility of the formation of negative heavy ions
in the chamber, a process in which electrons become attached to a neutral gas atoms or molecules. The
consequence of such electron attachment is the formation of slow moving negative ions, thereby altering the
speed and shape of the signal formation.
The mechanisms of electron attachment, described by Bloch and Bradbury [1935] and Herzenberg [1969],
and summarized by Huk et al. [1988], constitute a basic two-step process. Electrons come into contact with
an electro-negative molecule to form an excited negative ion

Y + e− → Y −∗ , (9.41)

where Y represents the electro-negative gas molecule. The excited electro-negative molecule may then
deexcite through re-emission of the electron

Y −∗ → Y + e− , (9.42)

or become stabilized by emission of photon

Y −∗ → Y − + γ. (9.43)

If the excited gas molecule releases the electron, the effect of electron attachment is basically nullified.
However, if the gas molecule becomes stabilized, then the electron charge carrier is converted into a slow
moving negative ion, with a decreased mobility by three or more orders of magnitude. Often, these parasitic
gases are contaminants in the host detection gas X. The negative ion in the excited state may instead collide
with the host detection gas such that

Y −∗ + X → Y + X + e− , (9.44)

or become stabilized by,


Y −∗ + X → Y − + X ∗ . (9.45)
The average probability of forming negative ions is a function of the electron attachment coefficient Ca
[Compton and Langmuir 1930], which is the average probability that a single collision causes an electron to
attach to an atom or molecule and can be expressed as

Ca = λe fV N σ at . (9.46)

Here N is the atomic density of the gas for the species being considered, fV is the volume fraction of that
gas in the chamber gas, and σ at is the average electron capture cross section. Unfortunately, there appears
Sec. 9.2. Electrons and Ions in Gas 319

Table 9.3. Electron attachment coefficients Ca in various gases. From [ Korff


1946; Loeb 1929]. Gases that have practically zero values for Ca include He,
Ne, Ar, Kr, Xe, H2 , N2 and CH4 [Loeb 1929, 1939].

Gas Ca Gas Ca Gas Ca

Air 5.0 × 10−6 C2 H 6 4.0 × 10−7 H2 O 2.5 × 10−5


BF3 1.24 × 10−8 CO 6.25 × 10−9 N2 O 1.64 × 10−6
C2 H 2 1.28 × 10−7 CO2 6.2 × 10−9 NH3 1.01 × 10−8
C2 H 4 2.13 × 10−8 Cl2 > 5.0 × 10−4 O2 2.5 × 10−5

Table 9.4. Electron attachment rate coefficients αI for O2 in various Ar/CH4 gas mixtures
as measured by Huk et al. [1988]. The samples had 200 ppm O2 added and the measurements
were conducted at a pressure of 4 bar.

Ar/CH4 – 90%/10% Ar/CH4 – 80%/20%

E/P ve αI E/P ve αI
V cm−1 bar−1 cm/μs μs−1 V cm−1 bar−1 cm/μs μs−1

100 5.36 0.048 ± 0.003 100 5.54 0.103 ± 0.006


138 5.45 0.034 ± 0.003 138 6.61 0.098 ± 0.007
163 5.32 0.029 ± 0.003 163 6.91 0.089 ± 0.007
200 5.07 0.024 ± 0.003 200 7.08 0.074 ± 0.007
250 4.70 0.019 ± 0.003 250 7.10 0.069 ± 0.007

to be some discrepancy regarding this simple definition, because the designation of “attachment coefficient”
has been assigned to various dimensioned numbers in the literature [Huk et al. 1988; Sitar et al. 1993]. In
the present work, the interaction coefficient ψI is defined as a function of the attachment coefficient, such
that [Sitar et al. 1993]
fV N σ at ω e Ca ω e fV N Ca ωe σm
ψI ≡ = = , (9.47)
ve λe ve ve
in which the last result is obtained from Eq. (9.21).
The attachment rate coefficient is defined as the rate at which electrons are attached to gas molecules
(atoms), per unit time, and is a function of gas pressure and electric field. It is defined as

Ca ω e
αI = ψI ve = . (9.48)
λe
In Table 9.3 values of the attachment coefficient are given, and in Table 9.4 attachment rate coefficients for
Ar/CH4 are listed for several reduced potentials.
Consider a cloud of electron-ion pairs produced with density Np at some location x from the anode within
a planar gas chamber of width d. Under bias, the electrons drift towards the anode and the positive ions
towards the cathode. To be collected, the electrons must drift a distance x over the time t = x/ve and the
positive ions must drift a distance d − x over the time (d − x)/vion . As the electrons drift, they are lost to
electron attachment described by
Ne (x) = Np e−ψI x , (9.49)
or, equivalently,
Ne (t) = Np e−αI t . (9.50)
320 Gas-Filled Detectors: Ion Chambers Chap. 9

Common detector gases, such as Ar and CH4 , have relatively low values for Ca , and Staub [1953] states
that Ar, CO2 , H2 , He and N2 have attachment coefficients that are very small, a statement supported in
part by data [Loeb 1929]. However, contamination in the detection gas from O2 or water vapor can increase
electron attachment and compromise performance [Staub 1953; O’Kelly et al. 1960; Huk et al. 1988]. Overall,
it is usually best to avoid using gases, or gas mixtures, in which a constituent has a fairly high value of Ca .
Further, care should be taken to ensure that the detector gas does not become contaminated with impurities
having large values of Ca , such as O2 or water vapor.

Example 9.1: In the operation of a Ar-filled ion chamber, operated with an electric field of 300 V cm−1 ,
it was discovered that the chamber is contaminated with 1% O2 . The chamber is operated at 20◦ C with
pressure of 1 atm. What is the expected electron attachment fraction per unit differential travel distance in
the chamber?

Solution:
From Fig. 9.5 the interpolated value (from the data) of the characteristic energy K is 3.0 eV, and is the
effective kinetic energy of free electrons in the electric field. From Eq. (9.35) (or Fig. 9.6) the drift speed is
3.6 × 105 cm s−1 , and from Fig. 9.4, the momentum transfer cross section is 4.2 × 10−16 cm2 . Also, from
Table 9.3, the capture coefficient for O2 is Ca is 2.5 × 10−5 , while that for Ar is essentially zero (Ca  0).
The average thermal speed is
 <
2K 2(3 eV)(1.6 × 10−19 J/eV)
ωe = =
me 9.1 × 10−31 kg
= 1.027 × 106 m s−1 = 1.027 × 108 cm s−1

The molecular density of O2 in the chamber is f NO2 = f ρO2 Na /AO2 . From Table 9.1, ρO2 = 1.33
mg/cm3 at 293 K and 760 torr. Thus,

(6.022 × 1023 mol−1 )


fV NO2 = (0.01)(1.33 × 10−3 g cm−3 ) = 2.50 × 1017 cm−3 .
32 g/mol

Then from Eq. (9.47) the interaction coefficient is


fV NO2 Ca ω e σm
ψI =
ve
(2.50 × 1017 cm−3 )(2.5 × 10−5 )(1.027 × 108 cm s−1 )(4.2 × 10−16 cm2 )
=
(3.6 × 105 cm/s)
= 0.7497 cm−1 .

Hence
Ne (x) −1
1− = 1 − e−ψI x = 1 − e−(0.7497 cm )(1 cm) = 0.5275.
Np
This results means that for every centimeter traveled by the electrons in the chamber gas, 52.75% of the
electrons become attached to the O2 molecules.

Although the average number of collisions per electron in a gas chamber varies with chamber size, gas
pressure, and applied electric field, Korff [1946] quotes the average number of collisions per electron per
detection event as approximately 105 . The average probability for electron attachment can be estimated
by multiplying the number of collisions by Ca . Hence, for those gases with Ca < 10−5 , the probability of
electron attachment is minimal. However, for gases with Ca > 10−5 , electron attachment can occur, thereby
slowing and distorting the electrical signal from the detector. The number of collisions expected for a single
Sec. 9.3. Recombination 321

electron traversing a chamber can be estimated from published values [Staub 1953], with the mean free path
generally ranges between 0.5 μm to 3.0 μm. Some halogen gases have relatively high values for Ca , as do O2
and water vapor.
9.3 Recombination
After the formation of electron-ion pairs, it is possible that some electrons recombine with positive ions
before they are separated by drift and diffusion. There are three basic types of recombination described
in the literature [Wilkinson 1950], namely columnar recombination, volumetric recombination, and prefer-
ential recombination.7 Columnar recombination occurs from the localized formation of a relatively dense
cloud of ion pairs around the trajectory of, for instance, an alpha particle in the detector gas. Electrons
recombine with positive ions, but generally not with their original parent atoms. Volumetric recombination
is the recombination of positive and negative ions produced by unrelated ionizing interactions. Preferential
recombination occurs when an electron attaches to a neutral atom and, subsequently, recombines with the
parent positive ion from whence the electron came, or, less probably, the electron recombines immediately
with its original parent atom.8
Note that recombination occurs only if the electrons and positive ions are locally close enough to enable
the process to occur. The product n− n+ is the combined localized charge carrier concentration within the
gas chamber. The larger this concentration, the greater is the rate of recombination. Even under low electric
field conditions, the diffusion of electrons is much higher than that of positive ions, and rapid separation
can be expected; hence, the effect of electron-ion recombination is typically minor. Recombination is less
prevalent in gases that have small electron interaction coefficients than found with electro-negative gases.
However, in gases that form heavy negative ions, through electron attachment for instance, recombination
may cause significant charge carrier losses.
9.3.1 Columnar Recombination
Columnar recombination is of most concern for gas-filled detectors operated in pulse mode, because the back-
ground or interaction rate under most situations is usually not high enough to cause appreciable volumetric
recombination. Columnar recombination is almost entirely caused by the recombination of positive and
negative heavy ions; therefore, those detector gases that do not suffer from electron attachment have mini-
mal columnar recombination. However, gases that have components that do have large electron attachment
coefficients, such as air, alcohols, or contaminated gases, can have appreciable columnar recombination.
Jaffé [1913] developed a theory for columnar recombination based on gases that have appreciable electron
attachment coefficients, in which the fraction of ions escaping recombination is described by
N∞ 1
F (E) = =  . (9.51)
No βN o π
1 + 8πD S(z)
ion z
Here β is the recombination coefficient, No is the initial number of electron-ion pairs in the ionization path
(eip density), N∞ is the number of ions that escape recombination, Dion is the ion diffusion coefficient, and
  ∞
1 e−S dS
S(z) = <  . (9.52)
π 0 S
S 1+
z

7 Loeb [1939] suggests as many as five types of recombination.


8 Inthe strictest sense, preferential recombination is the only true recombination of the many types, in that an electron stripped
from an atomic nucleus recombines back with its original parent atom. In the other two cases mentioned, columnar and
volumetric recombinations, electrons combine with any random positive ions, other than their original parents.
322 Gas-Filled Detectors: Ion Chambers Chap. 9

The substitution   
π iπ (1) iz
f (z) = S(z) = ez/2 H0 ( ), (9.53)
z 2 2
yields
N∞ 1
F (E) = = . (9.54)
No βN
1 + 8πD o f (z)
ion
(1)
where H0 is a Hankel function of the first kind of order zero,9 listed [Jahnke and Emde 1945] and plotted
elsewhere [Zanstra 1935]. The variable z is [Loeb 1939]
 2
1 Eμb sin θ
z= , (9.55)
2 Dion
where θ is the angle between the ionization track and the applied electric field, μ is the ion mobility, K1 is a
constant, E is the applied electric field and P is the gas pressure in atm. With the substitution z = 2x into
Eq. (9.53) and Eq. (9.55), Diebner [1931] shows that
 
x iπ (1)
f (x) = e H0 (ix), (9.56)
2
and is approximated by  
x 2 1.122
f (x) ≈ 2.303 1 + ex log10 , (9.57)
2 x
for x < 0.1, thereby providing a straightforward method to evaluate Eq. (9.51) as a function of x. However,
these equations, Eqs. (9.51) to (9.57), are all very interesting, but, without knowledge of b, F cannot be
directly evaluated.10 The evaluation method developed by Zanstra [1935] expresses Eq. (9.51) as,
N∞ I 1
F (E) = = = . (9.58)
No Io 1 + gf (x)
where I is the measured current, Io is the current without recombination, and
βNo
g= . (9.59)
8πDion
Rearranging terms, Eq. (9.58) can be rewritten as
1 1 gf (x)
= + . (9.60)
I Io Io
Zanstra [1931] asserts that, provided g is constant, Eq. (9.60) will yield a linear response. At f (x) = 0, the
condition I = Io is satisfied; hence by plotting 1/I vs f (x) and extrapolating to the ordinate intercept at
f (x) = 0 then Io can be obtained. This method was confirmed with satisfactory results by Clay [1939] and
Greening [1964]. For x > 10, Eq. (9.56) can be approximated by [Boag 1966]

π
f (x) ≈ . (9.61)
2x

9 Hankel (1)
functions are otherwise known as Bessel functions of the third kind (or Weber functions). Here H0 (z) = J0 (z)+iY0 (z),
where J0 (z) and Y0 (z) are Bessel functions of the first and second kind, respectively.
10 An average value of the product b sin θ was used for the work [Jaffé 1913].
Sec. 9.3. Recombination 323

Substituting Eq. (9.55) and Eq. (9.61) into Eq. (9.58) yields,
N∞ 1
=    . (9.62)
No βNo 2Dion π 1/2
1+
8πDion Eμb sin θ 2
Rearranging terms yields, and acknowledging that No ∝ Qo ,
  
1 1 β 2Dion π 1/2 1 1 C1
= + so that = + , (9.63)
N∞ No 8πDion Eμb sin θ 2 Q Qo Vo

where Q is the measured charge, Qo is the actual charge liberated, 1/Q


Vo is the applied voltage, and C1 is constant, resulting in a lin-
ear equation identical to that expressed by Attix [2004]. Hence, 1/Q2
for relatively high applied voltages, the inverse of the measured
charge Q can be plotted against measured values on the right side of
Eq. (9.63), as shown in Fig. 9.10. Extrapolating back to the origin 1/Q1
where C1 /Vo = 0, the actual value of a Qo can be found. 1/Qo
There are a few trends, perhaps obvious, that can be seen from
Eq. (9.51). First, columnar recombination increases with the den- 1/V
sity of No and the recombination coefficient β. Second, the recom- 1/V1 1/V2
bination decreases with larger diffusion coefficients Dion . Finally,
perhaps not so obvious from Eq. (9.51), but affirmed by Eq. (9.63), Figure 9.10. Graphic depiction of a
method to determine the correct Qo in the
columnar recombination decreases as the applied voltage is increased presence of columnar recombination from
or gas pressure is decreased. 1/Q = 1/Qo + C1 /Vo .

9.3.2 Volumetric Recombination


Volumetric recombination occurs upon irradiation of a gas medium in high radiation fields, such that negative
and positive ions encounter oppositely polarized charge carriers generated from multiple random events.
The volumetric rate at which negative charges, with concentration n− , are recombined with the positive
charges, with concentration n+ , thereby reducing both n− and n+ , is −βn− n+ , where β is the recombination
coefficient. Loeb [1939] quotes βe  2 × 10−10 cm3 s−1 for electron-ion pairs in Ar at 1 atm, and Rossi and
Staub [1949] makes the claim that βe is similar for most detector gases. The value of β is much larger if

the negative ions are not electrons, but instead negatively charged heavy ions, where βion ranges between
−6 3 −1 −6 3 −1
0.9 × 10 cm s − 1.7 × 10 cm s at 1 atm [Loeb 1929].

Effects of Diffusion and Recombination in an Ion Chamber


Consider the one-dimensional ion chamber shown in Fig. 9.11 whose gas is uniformly and constantly irradiated
such that So electron-ion pairs are created per unit volume per unit time. The intensity of the irradiation is
sufficiently high that the chamber is operated in the current mode. In this section three cases are considered:
(1) no diffusion or recombination effects, (2) only diffusion is important, (3) only recombination is important.
In the following analysis the approach taken by Rossi and Staub [1949] is used.

Case (1): No Diffusion or Recombination Effects


The positive and negative current densities j± formed, respectively, by the positive and negative ion drift
velocities v± caused by the electric field are given by

∇•j± = ±qe So . (9.64)


324 Gas-Filled Detectors: Ion Chambers Chap. 9

Equivalently, in terms of the ion concentrations

j± = ±qe n± v± . (9.65)

For the one-dimensional case of Fig. 9.11, the ion speeds are

v± = ±iv ± , (9.66)
+ and the current densities are

j± = ij ± , (9.67)

where j ± and v ± are the absolute values, respectively. Substitu-


0 x d
tion of Eq. (9.65) into Eq. (9.64) and use of the magnitudes v ±
Figure 9.11. Uniform irradiation of a pla- yields the following differential equations for the steady-state ion
nar configuration gas-filled ion chamber. Vol-
concentrations
umetric recombination increases as the source
dn± (x)
term S◦ , the production of electron-ion pairs, v± = ±So . (9.68)
is increased. dx
The general solution of these equations is
So
n± (x) = ± x + C±, (9.69)

where C ± are arbitrary constants that can be determined from the boundary conditions n+ (0) = 0 and
n− (d) = 0. In this manner, the concentration profiles are found to be

So So
n+ (x) = x and n− (x) = (d − x). (9.70)
v+ v−
In terms of the magnitudes v ± and j ± the current densities for the geometry of Fig. 9.11 are

j ± = qe n± (x)v ± , (9.71)

so that
j = j + + j − = qe [v + n+ (x) + v − n− (x)] = qe So d (9.72)
Finally, multiplication of j by the area A of the electrodes gives the steady-state saturation induced current

Is = qe So Ad. (9.73)

Case (2): Ion Drift with Diffusion


When diffusion caused by thermal agitation becomes appreciable, some ions near the electrode of the same
sign reach that electrode and are neutralized. This reduces the number ions that drift towards their collecting
electrode and, hence, reduces the induced current.
To quantify this effect, add diffusion to the previous analysis. Equation (9.64) still holds but Eqs. (9.65)
become
j+ = qe n+ v+ − qe D+ ∇n+ and j− = −qe n− v− + qe D− ∇n− . (9.74)
For the one-dimensional case of Fig. 9.11 and use of absolute values these equations yields

dn+ (x) dn− (x)


j + (x) = qe n+ (x)v + − qe D+ and j − (x) = qe n− (x)v − + qe D− . (9.75)
dx dx
Sec. 9.3. Recombination 325

Equation (9.64), as before, gives

dj ± (x)
= ±qe So or j ± (x) = ±qe So x + C1± . (9.76)
dx
where C1± are constants of integration. Equating the right-hand sides of Eqs. (9.75) and (9.76) gives, after
rearrangement,
dn+ (x) v+ So ?+ ,
= + n+ (x) − + x + C 1 (9.77)
dx D D
− −
dn (x) v So ?− ,
= − − n− (x) − − x + C 1 (9.78)
dx D D
?± = C ± /D± .
where C1 1
The most general solutions of Eqs. (9.77) and (9.78) are
+
x/D+ So x
n+ (x) = C2+ ev + + C3+ , (9.79)
v+

x/D− So x
n− (x) = C2− e−v − − + C3− , (9.80)
v
where C2± and C3± are arbitrary constants. To evaluate these four constants, use the four boundary conditions
n± (0) = 0 and n± (d) = 0. With these conditions the concentration profiles are found to be
 
v + x/D+
S o S o d 1 − e
n+ (x) = + x − + , (9.81)
v v 1 − ev+ d/D+
 − −

− So So d 1 − e−v x/D
n (x) = − − x + − . (9.82)
v v 1 − e−v− d/D−

For most practical ion chambers v ± d/D± are large numbers so that Eqs. (9.81) and (9.82) can be
approximated as
So So d + +
n+ (x)  x − + e−v (d−x)/D , (9.83)
v+ v
So So d − −
n− (x)  − (d − x) − − e−v x/D . (9.84)
v v
To obtain the current densities, substitute Eqs. (9.83) and (9.84) into Eqs. (9.75) to obtain
D+ D−
j + (x)  qe So x − qe So and j − (x)  qe So (d − x) − qe So . (9.85)
v+ v−
Finally, the induced current is seen to be
D+ D−
I = A(j + + j − )  qe So Ad − qe So A + . (9.86)
v+ v−
Thus, the decrease in the saturation current Is due to diffusion effects is

δIs  D+ D−
−  + . (9.87)
Is diffusion v+ d v− d
326 Gas-Filled Detectors: Ion Chambers Chap. 9

Figure 9.12. The relative charge collection 1 − (βRSo )/(6v+ v− ) for


air as a function of the electric field. Here the distance d between
electrodes is in cm and qe So = 1 nA cm−3 . Values of the other variables
are calculated in Example 9.2.

Substitution of Eq. (9.34) into Eq. (9.87), which also applies to ions, gives

δIs  3kT : + ;
−  ξ + ξ− , (9.88)
Is diffusion 2qe V
where V is the applied voltage. For heavy ions, the difference between the characteristic energy and the
thermal energy is small, hence for both negative and positive heavy ions ξ  1, and

δIs  3kT
−  , (9.89)
Is diffusion qe V
from which it is seen that diffusion losses are negligible for high voltages. However, for electrons, the value of
ξ can be considerably higher, on the order of 200 or more for typical electric fields employed in ion chamber
operation. In this case 
δIs  3kT : − ;
−   ξe + 1 . (9.90)
Is diffusion 2qe V
This result shows that there can be electron losses from diffusion if the operating voltage is on the order of
only a few hundred volts. Raising the operating voltage minimizes diffusion losses.
Case (3): Effect of Recombination
Assume that diffusion losses are negligible so that the ion concentration profiles are given by Eqs. (9.70).
The induced current, with recombination effects, is thus
 d
I = Is − δIs = qe So Ad − qe A βn+ (x)n− (x)R dx, (9.91)
0

where R is the fraction of free electrons that produce heavy negative ions through electron attachment.
Substitution of Eqs. (9.70) into this result yields
 
δIs  βR d So2 x(d − x) βR So d2
− = dx = . (9.92)
Is recombination So d 0 v+ v− 6 v+ v−
Sec. 9.3. Recombination 327

From Eq. (9.87) it is seen that losses from diffusion decrease with increasing electrode spacing while,
from Eq. (9.92), losses from recombination are seen to increase with electrode spacing. Equation (9.87)
also indicates that diffusion losses are independent of the source term So , and are inversely proportional
to the ion drift speeds, which are proportional to the applied electric field. Equation (9.92) indicates that
recombination losses increase proportionally to the source term So and inversely to the drift speeds of the
charge carriers (or applied voltage). The electric field required to move the operation of the detector from the
recombination region into the ion chamber region increases with radiation exposure, i.e., with So , as depicted
in Fig. 9.12. For gases with negligible electron attachment and, consequently, relatively small recombination
losses, the recombination region spans a small range of voltages. Examples of such gases with little to
no recombination losses include Ar, CH4 , P-10 and diatomic forms of halogens. However, contamination
from electronegative gases, such as O2 , O, NO, OH, and Cl, can cause considerable recombination, thereby
extending the range of the recombination region. Equation (9.92) indicates that the recombination region
increases as the volumetric ionization increases, as shown in Fig. 9.12. Hence, as So increases, the applied
electric field must also be increased to transition from the recombination region into the ion chamber region.

Example 9.2: An open air ion chamber is irradiated with 662-keV gamma rays to produce qe So = 1 nA
cm−3 . The ion chamber’s aperture is 2.5 cm × 2.5 cm and the electrode spacing is 2.5 cm. The electrodes
are designed as squares, each being 2.5 cm × 2.5 cm. The chamber is operated at 300 volts. The saturation
speed of electrons in air at 760 torr is ve = 6.58 × 105 cm s−1 . What is the fractional loss of saturation
current due to recombination?

Solution:
The electric field across the chamber is E = 300 V/2.5 cm = 120 V/cm. For energies below 0.2 eV,
there is an unfortunate lack of data for the ratio D/μ (or K ) for oxygen, although it can be assumed from
available measurements that K < ∼ 0.2 eV [Huxley and Crompton 1974; Peisert and Sauli 1984]. Instead,
assume that ξ = 1 so that K = E e , thereby giving as a first approximation the average thermal electron
energy as 3kT /2. The characteristic energy is then

qe De 2E e
K = = = kT  .026 eV,
μe 3
which can be interpreted as the minimum thermal energy.11 From Fig. 9.4, the momentum transfer cross
section σm for O2 is  7 × 10−16 cm2 . Also, from Table 9.3, the capture coefficient for O2 is Ca is 2.5 × 10−5 .
The capture coefficient for N2 is essentially zero (Ca  0).
 <
2K 2(0.026 eV)(1.6 × 10−19 J/eV)
ωe = = = 9.56 × 104 m s−1 = 9.56 × 106 cm s−1
me 9.1 × 10−31 kg

The mean free path λe between scatters with O2 is estimated as a function of O2 density, namely λe =
1/(f N σm ), where na = f N . From Eq. (9.47),

Ca ω e C a ω e σm f N (2.5 × 10−5 )(9.56 × 106 cm s−1 )(7 × 10−16 cm2 )


ψI = = =
λe ve ve 6.58 × 105 cm s−1
273K
×(0.21)(2.7 × 1019 cm−3 ) = 1.34 cm−1 . (9.93)
293K
If, instead, K = 0.2 eV is used, then ψI = 3.72 cm−1 . Hence, it can be assumed that the interaction
coefficient lies between the two extremes, i.e., 1.34 cm−1 ≤ ψI ≤ 3.72 cm−1 . With such a high interaction

11 Typically,the characteristic energy is much higher than the minimum thermal energy. Use of the minimum thermal energy
serves to provide the minimum thermal speed ω e .
328 Gas-Filled Detectors: Ion Chambers Chap. 9

coefficient, essentially all electrons become attached to an ion within 1 to 2 cm of air; hence R  1. Now
assume that direct electron-ion recombination is negligible, leaving only heavy ion recombination between
negative and positive heavy ions. From Table 9.2, the positive ion and negative ion speeds are
760μ+
air E 1.36 cm2 300V
v+ = = = 163.2 cm s−1 ,
P Vs 2.5cm
760μ− E 1.87 cm2 300V
v− = air
= = 224.4 cm s−1
P Vs 2.5cm
For qe So = 10−9 A cm−3 , the number of electron-ion pairs So produced per unit volume per unit time is
6.25 × 109 cm−3 s−1 . Finally, assume a high recombination coefficient of 1.7 × 10−6 cm3 ion−1 s−1 [see data
from Loeb 1929]. Thus,

δIs βSo d2 (1.7 × 10−6 cm3 ion−1 s−1 )(6.25 × 109 ion pairs cm−3 s−1 )((2.5 cm)2 )
− = − + = = 0.3022.
Is 6v v 6(224.4 cm s−1 )(163.2 cm s−1 )
This result means that approximately 30% of the charge carriers are lost to recombination.

Equation (9.92) is at times written as a collection efficiency [Boag 1966]


Q βR So d2 βR Q∗o d4 1
f= =1− = 1 − = 1 − ζ2, (9.94)
Qo 6 v+ v− 6 qe μ+ μ− Vo2 6
where Q∗o is the true ionization rate (esu cm−3 s−1 ), qe is the unit electric charge (in esu),12 and Vo is the
applied voltage across electrode separation d, and
< *  + *  +
βR d2 Q∗o ∗ d2 Q∗o
ζ= = k , (9.95)
qe μ− μ+ Vo Vo

where k ∗ is a constant. Through comparisons of experimental observations, an accepted average value of k ∗ is


36.7±2.2 V s1/2 cm1/2 esu1/2 for air at STP [Greening 1964]. Other terms in Eq. (9.95) are defined as follows
[Attix 2004]: d is the plate separation (cm), Q∗o = qNo /vl t (esu/cm3 s), qe the unit electrical charge (esu)
= 4.8032 × 10−10 esu, No the number of ion pairs produced in the chamber volume, vl the chamber volume
(cm3 ), t the irradiation duration (s), Vo the applied potential (volts), β the recombination coefficient (cm3 /
ion s), μ− the mobility of negative ions (cm3 /V s), μ+ the mobility of positive ions (cm3 /V s), and R the
fraction of negative ions from electron attachment. It is assumed the irradiation time t is long by comparison
to the ion-transit time across the detector (∼ 1 ms). The solution Eq. (9.92), and also Eq. (9.94), are based
on the charge density distributions described by Eq. (9.70), which ideally form a linear dependence with
position. Boag [1966] points out that the solutions Eq. (9.92) and Eq. (9.94) overestimate the recombination
in an ion chamber and offer a correction altering Eq. (9.70) with the charge carrier collection efficiencies,
f So f So
n+ (x) = x and n− (x) = (d − x). (9.96)
v+ v−
Substitution into Eq. (9.91) yields
f 2ζ 2
f =1− , (9.97)
6
12 The esu, or statcouloumb, is a nearly defunct unit in the cgs system, with a conversion to the SI system, 1 C = 2.9979 × 109
statC or 1 statC = 3.3357 × 10−10 C.
Sec. 9.3. Recombination 329

which actually underestimates the recombination losses. The derivations by Mie [1904] and Greening [1964]
produce a geometric average between the two derivations of Eq. (9.92) and Eq. (9.97), namely,

f ζ2
f =1− , or (9.98)
6
1
f= . (9.99)
ζ2
1+
6
Eq. (9.99) is accurate for d between 0.5 cm up to 8 cm provided that f ≥ 0.7. Rearranging terms with the
substitution qe No /vl t = Q∗o , Eq. (9.99) reduces to the linear equation

1 1 k ∗2 d4 1 C1
= + = + 2, (9.100)
Q qe No 6vl tVo2 Qo Vo

where C1 = k ∗2 d4 /6vl t is constant. Eq. (9.99) can be plotted to 1/Q


determine the true charge collection efficiency f , or the true value
of Qo , as shown in Fig. 9.13. Hence, by measuring the current, or 1/Q2
charge, at two different operating voltages, a line can be projected
through the ordinate at 1/V 2 = 0 to determine the value 1/Qo.
Equation (9.100) also holds true for cylindrical and spherical ion 1/Q1
chambers, although the device dimensions, and therefore ζ, must be 1/Qo
altered. For cylindrical detectors, in which a is the inner electrode
wire radius (usually the anode) and b is the outer wall electrode 1/V
2
radius (usually the cathode), one has 2 2
1/V1 1/V2

∗ [(b − a)κcyl ]
2
Q∗o Figure 9.13. Graphic depiction of a
ζcyl = k (9.101)
Vo method to determine the correct Qo in the
presence of volumetric recombination from
where 1/Q = 1/Qo + C1 /Vo2 .
    1/2
b+a b
κcyl = ln . (9.102)
2(b − a) a
For spherical detectors, in which a is the inner electrode wire radius and b is the outer wall electrode radius,
zeta is given by 
∗ [(b − a)κsph ]
2
Q∗o
ζsph = k (9.103)
Vo
where   1/2
1 b a
κsph = +1+ . (9.104)
3 a b

9.3.3 Preferential Recombination


Preferential recombination occurs when a liberated electron recombines with its original parent ion. The
process can occur when a heavy negative ion, formed through electron attachment, remains in close proximity
of the positive parent ion. The probability that preferential recombination occurs is [Onsager 1938]

−qe2
Ppr = 1 − exp , (9.105)
4πo ds kT
330 Gas-Filled Detectors: Ion Chambers Chap. 9

where ds is the distance between the negative and positive ions. Preferential recombination occurs when the
electrostatic attractive forces of the negative and positive ions overcome the thermal Brownian motion of
the ion-pair, i.e., when
qe2 > 3
kT. (9.106)
4πo ds ∼ 2
Wilkinson (1950) points out that preferential recombination is generally unimportant for ion chambers
operated under typical gas pressures. Regardless, the effect of preferential recombination is to remove charge
carriers from the signal formation process, the same as columnar and volumetric recombination. Hence, its
effect is nearly indistinguishable from other forms of recombination, except, perhaps, at high gas pressures
where D± becomes small. Loeb [1939] suggests that gases with high attachment coefficients, such as O2 ,
Cl2 , SO2 , and CO2 , may experience preferential recombination for pressures above 5 to 10 atm.

9.4 Ion Chamber Operation


ionizing Perhaps the simplest gas-filled detector is the
electron-ion radiation ion chamber. There are many configurations
pairs
of ion chambers, and they are operated in Re-
Vin Vout gion II of the gas curve. The detection method
A is simple. Ionizing radiation, such as charged
-
++ - particles or energetic photons, enter a region
- +
+
+ - - filled with a gas, such as Ar or air. The cham-
+V0
ber has electrodes across which a voltage is
applied. As the radiation interacts with the
x gas, electron-ion pairs are created, depicted in
Fig. 9.14, whose number is proportional to the
0 x1 x0 x2 d radiation energy absorbed. The voltage ap-
plied across the electrodes causes the negative
Figure 9.14. Depiction of an ion chamber of planar design.
electrons to separate from the positive ions
and drift across the chamber volume. Elec-
trons or negative ions drift towards the anode, and positive ions drift towards the cathode. Such charge
motion induces current to flow in the external circuit.
Typically, this induced current is sensed by either directly measuring the current or by first storing the
charge in a capacitor and then measuring the resulting voltage across the capacitor. The first case is referred
to as current mode operation and the second case is pulse mode operation. Current mode operation is used
in high radiation fields, and the magnitude of the current measured gives a relative measure of the radiation
field. Pulse mode is used for lower radiation fields, and allows each radiation particle interacting in the
chamber to be counted. The voltage produced by the ion chamber detector is the input voltage to the
amplification circuitry, and hence, is referred to as Vin . The shaped voltage pulse exiting the accompanying
amplification circuits is referred to as the output voltage Vout .
Ion chambers come in many forms: they can be used for reactor power measurements, in which the
radiation field is very high, and for small personnel dosimeters, in which the radiation levels are typically
very low. Although simple in concept, two main problems occur when the ion chamber is operated in pulse
mode, namely, (1) the measured signal is small due to relatively few electron-ion pairs produced by a single
radiation particle and (2) the time to form a signal can be relatively long due to the slow motion of the
heavy positive ions. To ameliorate this second problem, an RC circuit is often connected to an ion chamber
to reduce the time constant of the system, thereby reducing the time response. Consequently, the capacitor
usually discharges before all of the ions are collected.
Sec. 9.4. Ion Chamber Operation 331

9.4.1 Planar Ion Chambers


A planar ion chamber of the design shown in Fig. 9.14 is operated with positive potential V0 applied across
the electrodes separated by distance d. A radiation particle deposits energy at location x0 in the chamber
and creates a cloud of electron-ion pairs. The number of electron-ion pairs produced is proportional to the
energy deposited within the detector gas by the radiation particle.
Current Mode Operation
A simple current mode arrangement for measuring radiation
interactions is shown in Fig. 9.15. Radiation interactions in the I
chamber create electron-ion pairs, which are drifted across the - - current
chamber to their respective collecting electrodes by the applied - - C meter
+ + D
voltage. + +
One method used to measure the energy deposited by radi- V0
ation interactions within an ion chamber is to directly measure
the current. This action can be accomplished by inserting a
current meter into the circuit, as depicted in Fig. 9.15. Be-
cause electron speeds are much higher than ions, the current is Figure 9.15. Current mode operation of an ion
highest while electrons are in motion. The measured current is chamber.
defined as
Q qe Eve qe Evion qe E qe E
I= = + = + , 0 < t ≤ te . (9.107)
t wΔxe wΔxion wte wtion
and
qe E
I= , te < t ≤ tion , (9.108)
wtion
where E is the energy deposited in the detector, w is the average energy the radiation particle must deposit
in the gas to produce an electron-ion pair, and te and tion are the electron and ion extraction or sweep-out
times, respectively.

Example 9.3: Calculate the initial instantaneous current measured from an energy deposition of 1 MeV
by a radiation particle in an ion chamber operated with pure Ar gas at 1 atm. The distance d between the
electrodes is 2 cm with an applied bias of 200 volts. The interaction occurs at x0 = 0.5d.

Solution:
From Table 9.1, the average energy required to produce a electron-ion pair in Ar is 26 eV. For an electric
field of 200 V, the reduced electric field at 1 atm (760 torr) is
E 200 V
= = 0.132 V cm−1 torr−1 ,
P (2 cm)(760 torr)
From Eq. (9.35), the electron drift speed in argon is
3.64(E /P ) + 114.6(E /P )2
ve =
1 + 12.7(E /P ) + 304.33(E/P )2
3.64(0.132 V cm−1 torr−1 ) + 114.6(0.132 V cm−1 torr−1 )2
=
1 + 12.7(0.132 V cm−1 torr−1 ) + 304.33(0.132 V cm−1 torr−1 )2
= 0.364 cm/μs = 3.64 × 105 cm/s. (9.109)
From Table 9.2, the positive ion mobility is 1.7 cm2 V−1 s−1 , and from Eq. (9.30)
+
vion = μ+ 2
ion E = (1.7 cm V
−1 −1
s )(100 V cm−1 ) = 170 cm/s.
332 Gas-Filled Detectors: Ion Chambers Chap. 9

The initial current is mainly from electron motion; hence, the extraction time over distance d − x0 = 1 cm is
1 cm
t= = 2.75 μs.
3.64 × 105 cm s−1
Thus, the initial current is
Q (106 eV)(1.6 × 10−19 Coulombs)
I=  = 2.24 nA.
t (26 eV/e-ion pair)(2.75 × 10−6 seconds)
After the electrons are collected, the positive ions are collected with an extraction time of (1 cm)/(170 cm
s−1 )= 5.88 ms. Thus the current decreases to
(106 eV)(1.6 × 10−19 Coulombs)
I= = 1.05 pA,
(26 eV/e-ion pair)(5.88 × 10−3 s)
decreasing to zero after all ions are collected.

Ion chambers are frequently used in high radiation environments in which pulse processing is not possible
because of unacceptable pulse pile-up and dead time losses. However, under low irradiation conditions, the
induced currents can be very small and difficult to measure. Thus under these conditions it is more practical
to employ pulse processing methods and to operate the detector in pulse mode.
Pulse Mode Operation
A planar ion chamber is operated with positive potential V0 applied across the electrodes separated by
distance d as shown in Fig. 9.14. As before, a radiation particle deposits energy at location x0 in the
chamber and creates a cloud of electron-ion pairs. The motion of these mobile charges induces current to
flow across a coupling capacitor in which the charge is stored and measured as a voltage V = Q/C. The
pulse shape provided by the detector Vin is determined by several physical parameters, including the type
of gas, chamber, line and coupling capacitances, and the detector load resistor. Three operating cases are
considered in the following analyses.
Case 1: No Electron Attachment Here it is assumed that the gases chosen for the ion chamber have negligible
electron attachment coefficients; hence, the charge carriers are restricted to electrons and positive ions. The
solution for current and charge induction for a planar detector was developed in Chapter 8, where it was
found (see Eq. (8.43))  
x0 − x1  x2 − x0 
ΔQ = qe No + . (9.110)
d  + d −
ions e
Because the mobility of electrons in gas far surpasses that of the heavy ions, the saturation drift speed
of electrons ve = μe E is always much higher than the drift speeds of ions vion = μion E, i.e., ve vion .
Consequently, the electron sweep-out time te = (x2 − x0 )/ve is much smaller than the ion sweep-out time
tion = (x0 − x1 )/vion , i.e., te  tion .
If t is measured from the time of the ionizing event, the induced charge changes in time as the charge
carriers are swept out of the chamber. From Eq. (9.111) the induced charge is first seen to vary as
qe N o t
ΔQ(t) = [vion + ve ] , 0 < t ≤ te . (9.111)
d
Regardless of the location of x0 , the total charge induced at time te is
qe No te
ΔQ(te ) = [vion + ve ] , (9.112)
d
Sec. 9.4. Ion Chamber Operation 333

Figure 9.16. Normalized induced charge input from a planar ion


chamber as a function of interaction location d − x0 . Depicted is the
case in which ve = 100vion .

which, because ve vion , can be approximated as

ve te d − x0
ΔQ(te )  qe No = qe No . (9.113)
d d
After the electrons are rapidly collected, the positive
ions continue to drift across the chamber at a much lower
speed, so the collected charge is

vion t d − x0
ΔQ(t) = qe No + , te < t ≤ tion .
d d
(9.114)
Finally, for t > tion all the charge has been collected and
ΔQ remains constant at

x0 d − x0
ΔQ(t) = qe No + = qe No , t > tion .
d d
(9.115)
The induced charge input for a planar device is shown
in Fig. 9.16. Typically, vion for normal operating volt- Figure 9.17. Normalized output voltage Vout for vari-
ous interaction locations d−x0 in a planar ion chamber.
ages of an ion chamber is much too slow for pulse mode
operation, and the system RC network discharges the stored charge before all of the ions are collected. Con-
sequently, the induced charge applied to the detector shaping electronics is best described by Eq. (9.113), in
which the contribution of positive ions is mostly neglected. Also, the pulse height described by Eq. (9.113)
is dependent upon the initial location of the ionization cloud, i.e., the pulses are position dependent. The
electronic signals from ion chambers operated with gases having low electron attachment coefficients are
dominated by electron motion. As a result, ion chambers generate signals that are strongly dependent upon
the interaction location within the detector. Recall from Chapter 8 that V = Q/C. The time dependent
334 Gas-Filled Detectors: Ion Chambers Chap. 9

rise in voltage from an ion chamber with intrinsic capacitance C is, thus,

ΔQ qe N o t qe N o t
Vin (t) = = [vion + ve ]  ve . (9.116)
C Cd Cd
The ideal voltage output from a planar ion chamber, for an input
- - voltage Vin to the electronic circuitry, is depicted in Fig. 9.17. How-
- - C
+ +
+ +
D Cp R L Vin (t) ever, the ion chamber capacitance CD , line and stray capacitances Cp ,
and the load resistor RL connected to the voltage supply form an RC
network that introduces a time constant τ intrinsic to the detector.
V0 The equivalent circuit for the time dependent input from a planar ion
Figure 9.18. Equivalent circuit model chamber is depicted in Fig. 9.18, that, as discussed in Chapter 22, forms
for the time variant input voltage from a high pass differentiator circuit. The load resistor provides a leakage
an ion chamber. path to drain charge from the coupling capacitor between the detector
and the preamplifier circuit, without which the coupling capacitor would eventually saturate. If RL is too
small, current from the detector is drained too quickly and the resulting voltage is small. If RL is too large,
τ becomes large, causing pulse pile-up from consecutive radiation interactions and, eventually, causing the
coupling capacitor to saturate. The time dependent voltage from an ion chamber with intrinsic capacitance
C and load resistance RL is
qe N o t
Vin (t)  [vion + ve ] t exp − , (9.117)
Cd RC
Typically, the load resistor is chosen such that the time constant is much greater than the longest possible
electron collection time, while remaining shorter than the ion collection time, or tion RC te . As a
result, the intrinsic differentiator circuit has little discharge effect upon the electron induced current, yet
causes the coupling capacitance to discharge before the ions are collected. The effect of the RC time constant
upon Vin (t) is depicted in Fig. 9.19. The combined effects of position dependent charge collection and the
intrinsic system RC time constant lower the voltage pulse height from the ideal maximum. This difference
in the expected value is called the pulse height deficit, an example of which is shown in Fig. 9.19. The
magnitude of the pulse height deficit is a function of the RC time constant and the radiation interaction
location in the ion chamber.

Example 9.4: An ion chamber filled with pure argon at 1 atm is operated with the following parameters:
V0 = 200 volts; RL = 5 MΩ; C = 65 pF; d = 5 cm; x0 = 2 cm from the anode; deposition energy E = 5.5
MeV. What is the maximum input voltage pulse after the radiation interaction? Compare the answer to
that of an interaction occurring at x0 = 5 cm from the anode. Determine the pulse height deficit for both
cases.

Solution:
The time constant is τ = RC = 300 μs. From Table 9.1 the average energy to produce an electron-ion pair
in Ar is 26 eV, so that the total number of electron-ion pairs produced is

5.5 × 106 eV
N0 = = 211538 eip.
26 eV/e-ion pair

For τ → ∞, the expected input voltage is from Eq. (9.115)

ΔQ qe N0 (1.6 × 10−19 C)(211538 e-ion pairs)


Vin = = = = 0.5207 mV.
C C 65 × 10−12 F
Sec. 9.4. Ion Chamber Operation 335

Figure 9.19. Normalized input voltage Vin from a planar ion chamber,
where (d − x0 )/d = 0.7 and ve = 10vion . Comparison between systems
with different RC time constants is shown.

With an electric field of 200 V/ 5 cm = 40 V/cm, the reduced electric field at 1 atm (760 torr) is
E 200 V
= = 0.0526 V cm−1 torr−1 .
P (5 cm)(760 torr)
From Eq. (9.35), the electron speed in argon is
3.64(E /P ) + 114.6(E/P )2
ve =
1 + 12.7(E /P ) + 304.33(E/P )2
3.64(0.0526 V cm−1 torr−1 ) + 114.6(0.0526 V cm−1 torr−1 )2
= = 0.203 cm/μs = 2.03 × 105 cm/s
1 + 12.7(0.0526 V cm−1 torr−1 ) + 304.33(0.0526 V cm−1 torr−1 )2
From Table 9.2, the positive ion mobility is 1.7 cm2 V−1 s−1 , and from Eq. (9.30)
+
vion = μ+ 2
ion E = (1.7 cm V
−1 −1
s )(40 V/cm) = 68 cm/s.
The electron extraction time is
x0 2 cm
te = = = 9.85 × 10−6 s,
ve 2.03 × 105 cm/s
and the ion extraction time is
d − x0 2 cm
tion = = = 44.12 × 10−3 s.
vion 68 cm/s
Because te τ tion , the maximum input voltage is estimated from Eq. (9.117) at te as
qe No te
Vin (te )  − [vion + ve ] te exp − ,
dC RC
(1.6 × 10−19 C)(211, 538 e-ion pairs)
=−
(5 cm)(65 × 10−12 F)
  9.85 × 10−6 s
× 68 cm/s + 2.03 × 105 cm/s (9.85 × 10−6 s) exp − = 0.2016 mV.
300 × 10−6 s
336 Gas-Filled Detectors: Ion Chambers Chap. 9

The pulse height deficit is 0.5207 mV − 0.2016 mV = 0.3191 mV. By comparison, if the interaction occurred
at x0 = d, then the induced current is produced entirely from electron motion and te = 2.46 × 10−5 s. The
input voltage in this case is
qe No te
Vin (te )  − ve te exp − ,
dC RC
(1.6 × 10−19 C)(211, 538 e-ion pairs) 2.46 × 10−5 s
=− exp − = 0.4797 mV.
(65 × 10−12 F) 300 × 10−6 s
The pulse height deficit is 0.5207 mV − 0.4797 mV = 0.041 mV.

Although discussions on nuclear electronics are reserved for Chapter 22, to illustrate the consequence of
slow positive ion speeds, the following exposition is offered. The input voltage Vin (t) from a ion chamber is
commonly applied to a CR-RC preamplifier. The preamplifier consists of (1) a low-pass integrating/shaping
circuit that has an Ri Ci time constant τi , and (2) a high-pass differentiating/shaping circuit that has an
Ro Co time constant of τo . If it is assumed that the collection time for electrons is much less than the time
constant (te  τ ), and the time constant is much less than the collection time for the ions (τ  tion ), then
Eq. (9.113) can be approximated as a step input to the electronic circuitry. The observed output voltage
from the preamplifier circuit for a step input is,
τo
Vout (t)  Vin (t) e−t/τo − e−t/τi , (9.118)
τo − τi
Often, the time constant for input and output are equal, i.e., τo = τi . Substitution of Eq. (9.113) and
use of L’Hôpital’s rule13 yields
qe No ve te t −t/τ
Vout (t)  e t > te , (9.119)
Cd τ
where it is assumed that te is relatively small such that the input appears as a step input, and
qe No (d − x0 ) t −t/τ
Vout (t)  e . (9.120)
Cd τ
The normalized output voltages Vout as a function of interaction location d − x0 for monoenergetic ionizing
radiation particles are shown in Fig. 9.17, from which the responses are seen to be overwhelmingly position
dependent. As a result, a monoenergetic ionizing radiation source produces a continuous spectrum of signals
with varying amplitudes, thus, precluding the use of a planar ion chamber as an energy spectrometer.
Case 2: High Electron Attachment Consider the case in which the gas in the ion chamber has high elec-
tronegativity; in other words, the electrons become attached to neutral molecules almost immediately after
liberation. The induced charge now becomes
qe No t  + −
 qe No tE  + 
ΔQ = − vion + vion =− μion + μ−
ion . (9.121)
d d
The time dependent input voltage from the detector is
ΔQ qe N o t  + −

Vin (t) = =− vion + vion . (9.122)
C Cd
13 Although named after Guillaume François Antoine Marquis de L’Hôpital, evidently it was his tutor Johann Bernoulli who
discovered the rule (for pay), as indicated by communications between the two mathematicians [Dunn and Shultis 2012].
Sec. 9.4. Ion Chamber Operation 337

Because mobilities for positive and negative ions are only slightly different, the pulse mode signals produced
are small for typical operating voltages applied to ion chambers; however, they are much more consistent in
magnitude than the case in which electrons dominate. Nevertheless, there is some dependence of the pulse
magnitude on the energy deposited and the resulting induced signal formed from the drifting ions. Back-
ground and electronic noise further degrade the spectroscopic performance. Consequently the ion chamber
typically cannot be used for energy spectroscopy. However, these detectors can be used in current mode to
measure high radiation fields.
Case 3: Moderate Electron Attachment If the ion chamber is contaminated with an electronegative gas, the
electrons are lost by electron attachment according to Eq. (9.49) and Eq. (9.50). In pulse mode operation,
the positive ions and electrons are rapidly separated; hence, it is assumed that recombination is minimal.
Electrons lost from attachment to neutral molecules become slow moving negative ions. But if electrons are
the main contributor to the current, the instantaneous current produced at time t is
dQ qe No  −αI t  d − x0
I= =− ve e , t≤ = te , (9.123)
dt d ve
where αI is the electron interaction rate coefficient. Integration of Eq. (9.123) yields the time dependent
input voltage from the detector as
 t
qe No  −αI t   qe No ve
Vin (t)  − ve e dt = − (1 − e−αI t ) , t ≤ te . (9.124)
0 Cd Cd αI
Within the electron collection time te , the electrons have either attached to neutral molecules or have been
collected. The induced signal is position dependent, dominated by electron motion (unless αI is very large).
The observed slope of the time dependent signal decreases with t, thereby reducing the output signal below
that expressed by Eq. (9.116).
After the electrons have been collected, the positive ions continue to drift and produce an induced voltage
described by
qe N o t  +  x0
+
Vin (t) = − μion E , t≤ + = tion . (9.125)
Cd μion E

The heavy negative ions produced from electron attachment also continue to drift. Assuming that ve vion ,
the input voltage produced by the heavy negative ions is found to be (see Exercise Problem 9.7)
"   #
− qe No ve μ−
ion E e−αI te αI tμ−
ion E d − x0
Vin (t) = − t+ 1 − exp , t≤ − . (9.126)
Cd ve αI ve μion E
The total input voltage from the detector with moderate electron attachment is found by summing Eq. (9.124),
Eq. (9.125), and Eq. (9.126). An example is shown in Fig. 9.20.

9.4.2 Coaxial Ion Chambers


In Chapter 8, it was shown that the charge induction for a coaxial detector was a function of the inner
electrode diameter and the outer electrode diameter. The shape of the signal output changes significantly
depending upon the bias configuration. Typically, a positive voltage is applied to the inner electrode, as
shown in Fig. 9.21. The charge induction for electrons and positive ions is given by Eq. (8.79) which can be
written as   −1 "      #
r2 r2 r
ΔQ = qe No ln ln − ln 1 . (9.127)
r1 r0 r0
338 Gas-Filled Detectors: Ion Chambers Chap. 9

Figure 9.20. Normalized detector input voltage Vin (t) for an ion cham-
ber with moderate electron attachment. Shown is the case for ve = 50vion ,
xo = 0.5d and RC = ∞. V (t) is the sum of induced voltage from electrons
(Qe /C), positive (Q+ /C), and negative (Q− /C) ions.

Vin Vout The electric field for a cylindrical detector is given by


+V0 A Eq. (8.75), namely,

V0+ r2
E(r) = ln , (9.128)
r r1
r0 r’2
ionizing
radiation where V0 is the positive voltage applied to the inner electrode.
r’1 Because the electric field now varies with r, the drift speeds of
the charge carrier are position dependent such that
r1 -
++ - r2
- ++- V0 r2
+ -
v ± (r) = μ± E(r) = μ± ln . (9.129)
r r1
The minimum electron speed is at radius r2 , namely,
electron-ion
pairs − V0 r2
vmin = μ−
e ln . (9.130)
r2 r1
Figure 9.21. Depiction of an ion chamber of If the electron speed is much higher than the positive ion speed,
cylindrical design.
as is usually the case, then the electrons are swept out much
more rapidly than the ions, thereby contributing the most to the induced charge, as was found for the planar
case. Just after the electrons have been collected r1 = r1 and the positive ions have moved little, i.e., r2  r0 ,
the induced charge is, from Eq. (9.127),
  −1    
r2 r0 −1 r0
ΔQ(te ) = qe No ln ln = qe No [ln(R21 )] ln R21 , r0 ≥ r1 (9.131)
r1 r1 r2
where R21 is the ratio r2 /r1 . Reversal of the bias polarity yields the induced charge just after the electrons
Sec. 9.4. Ion Chamber Operation 339

(b)

(a)

Figure 9.22. The normalized induced charge ΔQ/(qNo ) just after the electrons have been collected
for a cylindrical ion chamber as a function of interaction location r0 and ratio R21 . In (a) positive bias
is applied to the inner electrode of radius r1 and the outer electrode at r2 is grounded. In (b) negative
bias is applied to the inner electrode with outer electrode grounded. Applying positive voltage to the
inner electrode has the clear advantage of producing larger signals over much of the detector volume.

have been collected


  −1    
r2 r2 r0
ΔQ(te ) = qe No ln ln = −qe No [ln(R21 )]−1 ln , r0 ≥ r1 . (9.132)
r1 r0 r2
The dependency of Vin (t) on radiation interaction location, the ratio r2 /r1 and the bias voltage polarity is
shown in Fig. 9.22.
The predicted electron drift speed is complicated by the fact that low energy (thermal) electrons, with
an average energy of 3/2kT , lose very little energy when colliding with a heavy ion. Hence, as an electric
field is applied to a gas, free electrons gain much higher energies than the average thermal energy. The ratio
between the electron characteristic energy (K ) and the thermal energy is denoted by the ratio ξ. As result,
the mobility of the electrons is not constant but is a function of the electric field. To develop the expected
time-dependent pulse shape from a coaxial ion chamber, the following semi-empirical relation is adopted for
the electron speed [Wilkinson 1950], namely,
 1/2
E
ve = C1 . (9.133)
P
Here C1 is an experimentally determined constant. This expression is valid for low values of reduced electric
fields.
The input pulse into the coupling electronics is
ΔQ(t)
Vin (t) =
, (9.134)
C
where C is the combined coupling and detector capacitance. Because the electron drift speeds are much
greater than those of the positive ion, the charge induction between 0 ≤ t ≤ te is dominated by electron
motion. From Eq. (8.44) for r2  r0 one has
 
−1 r0
ΔQ(t)  qe N0 [ln (R21 )] ln , (9.135)
re (t)
340 Gas-Filled Detectors: Ion Chambers Chap. 9

where r0 is the radial location of the initial ionization event and re (t) = r1 (t) is the electron cloud location
at time t. The electron drift speed changes with radial location as
1/2
dr C1 C1 V0
ve (r) = − = 1/2 E(r)1/2 = 1/2 . (9.136)
dt P P r ln (R21 )
Integration of this result gives
 r−e(t)  t 1/2
C1 V0
− r1/2 dr = dt (9.137)
r0 0 P 1/2 ln (R21 )
or
1/2
2 3/2 C1 V0
r − re3/2 (t) = 1/2 t. (9.138)
3 0 P ln (R21 )
The electron sweep out time te , i.e., when re (te ) = r1 , is found to be
& 1/2
3/2 3/2 3 C1 V0
te = r0 − r1 . (9.139)
2 P 1/2 ln (R21 )
Equation (9.138) can be solved for re (t) and combining this result with Eqs. (9.135) and (9.134) yields the
pulse height Vin (t) as a function of time, namely,
⎡ $ /2/3 ⎤
1/2
qN0 ⎣ln r0 − ln r03/2 − 3 C 1 V0 ⎦.
V (t) = − t (9.140)
C ln(R21 ) 2 P 1/2 ln(R21 )

The general voltage pulse height time response for coaxial ion chambers, with positive voltage applied to the
central wire, is shown in Fig. 9.23. Although the coaxial ion chamber pulses are still dominated by electron
motion, the coaxial geometry reduces the problem of widely varying position-dependent pulses that occurs
in planar ion chambers.

9.5 Ion Chamber Designs


Ion chambers have been used as radiation detectors from the time of Rutherford’s and Geiger’s invention
of the gas-filled radiation detector. Designs have been improved over the past 100 years to reduce leakage
current, stabilize output, and reduce the dependence on the position of the ionizing event. A list of specialized
ion chambers would be much too long to cover in the present work, but descriptions for many of these devices
can be found in the literature [Rossi and Staub 1949; Staub 1953; Price 1964; Boag 1966, 1986; Attix 2004;
Sauli 2014]. Presented here are several common designs encountered in radiation detection and measurement.
The profile of energy deposition in an ion chamber depends on the gas container, the type of gas and the
gas pressure. Penetrating radiation, such as gamma-rays, interact readily with the chamber walls, producing
energetic electrons (photoelectrons, Compton electrons, or, if Eγ > 1.022 MeV, electrons and positrons
from pair-production). These secondary electrons, if sufficiently energetic, can escape the walls and enter
the gas, thereby producing a cloud of electron-ion pairs. The response of the chamber to these secondary
electrons can be altered by lining the chamber with materials having of varying Z to change the probability a
gamma-ray interacts in the wall and the probability a secondary electron escapes into the gas. Gamma rays
can also interact directly with the chamber gas. Increasing gas pressure and the Z number of the detection
gas both increase the efficiency of the detector. Because ion chambers are usually designed to measure the
electrons produced by ionization, except in special cases, the contribution of the ion motion is minor. Hence,
the adverse effects that increasing gas pressure has on ion motion are of little consequence, and the electron
speeds remain high.
Sec. 9.5. Ion Chamber Designs 341

Figure 9.23. Normalized input voltage as a function of normalized time,


where t = 1 is the drift time between r2 and r1 and R21 = 500. Shown
are the cases in which a radiation interaction occurs at the cathode, and
at two different locations within the detector where r0 < r2 .

9.5.1 Basic Designs and Characteristics


Although an ion chamber is a simple concept, there are important design details that cannot be overlooked.
For instance, the insulators must be selected to reduce leakage current during operation in a radiation field.
The resistivity of the feedthroughs must be extremely high to reduce leakage current from moving around
the device from anode to cathode.
Planar Ion Chamber Designs
A simple planar ion chamber configuration and its equivalent
circuit are shown in Fig. 9.24. A voltage V0 is applied across resistive ion chamber resistive
the chamber volume and load resistor RL . Because the actual feedthrough feedthrough
IC
gas chamber resistance RC is extremely high, almost all of the
voltage is dropped across the chamber and very little across the
load resistor. As a result, most of the voltage is also dropped Vin
IL
across the insulating feedthroughs and the chamber body. The V0
resistance of the feedthroughs and chamber are represented by
RF , and the leakage current is IL = V0 /RF . The leakage cur-
rent can be reduced by using high resistance materials, thereby IC+ IL
IC
ensuring that RF is large and IL is small.
The detector input voltage becomes contaminated by the IL
leakage current, becoming Vin = (IC + IL )RL . The leakage
current adds white noise and can produce an incorrect assess- RF
ment of the radiation environment. To illustrate the problem, a V0 IRL = Vin
common ion chamber operated at the modest voltage of 100 V
requires the insulator feedthroughs have a combined resistance
Figure 9.24. (Top) Planar ion chamber. (Bot-
of 1016 Ω to keep the leakage current below 10−14 amp. By tom) The equivalent circuit model for the planar
comparison, the background current produced by cosmic rays ion chamber.
342 Gas-Filled Detectors: Ion Chambers Chap. 9

is on the order of 10−16 amp. Common high resistivity materials used for electrical feedthroughs include
Teflon ( 1025 Ω cm), quartz ( 7.5 × 1019 Ω cm) and alumina ( 1016 Ω cm).
Although the volumetric resistivity of many candidate materials is sufficiently high to serve as
feedthroughs, it is usually the surface leakage current that causes problems. The surface leakage is largely
dependent on the cleanliness of the surface and the ability of the insulator to absorb moisture. Scratches or
other surface damage can also increase surface leakage current. Many attractive high resistivity materials,
such as Teflon, undergo resistivity changes as a result of radiation damage. If the ion chamber is to be oper-
ated in high radiation fields, materials to be avoided include plastics, Teflon and, under some circumstances,
polystyrene. Many ceramic materials, such as alumina and quartz, appear to have much better radiation
resistance, and therefore are frequently used as feedthroughs for ion chambers.
guard
An interesting consequence of using plastics and
ring polystyrene, or other soft insulating materials, is the
ion chamber Rg generation of stress currents. Stress currents arise from
electron migration through the insulator when the ma-
R1 IC R2 terial is under high voltage. Although not an issue
IL2 for systems with detection currents greater than 10−13
amp, stress currents can become problematic for cham-
Rg I RL Vin
ber currents less than 10−14 amp. Thus, the stress cur-
IL1 V0 rent can determine the lower limit of sensitivity for the
IL1
ion chamber. Dielectric strength is a measure of the
electric stress required to abruptly move substantial
guard charge on or through a dielectric. Ceramic materials
IC ring such as alumina and quartz appear to have low stress
IL1 currents.
I-IC R I
2 One method to reduce bulk and surface leakage
IRL = Vin
R1 Rg through and around an insulator is to incorporate a
Rg
guard ring into the detector. A planar ion chamber
with a guard ring is depicted in Fig. 9.25, along with
V0
the equivalent circuit. The guard ring is placed around
Figure 9.25. (Top) Planar ion chamber with a guard ring. the collection electrode and grounded into the detector
(Bottom) The equivalent circuit model for the planar ion circuit, as shown in Fig. 9.25. The operating voltage
chamber with a guard ring. is applied across the chamber, and leakage current IL1
flows through (or around) the resistive feedthroughs
for the electrode, with resistance R1 , and guard ring, with resistance Rg . This leakage current IL1 bypasses
the loading resistor RL and instead returns to ground. Hence, the leakage current IL1 does not contribute
to Vin .
The voltage drop across the guard ring insulator and the collection electrode insulator is determined by
leakage current IL2 , as depicted in Fig. 9.25. However, because almost all voltage is dropped across the high
resistance of the ion chamber, the actual voltage drop between the guard ring and the collection electrode is
practically zero; hence, Vg−2 = IL2 (R2 + Rg )  0, meaning that the leakage current IL2 is practically zero
as well. As a result, the measured detector current has little contamination from leakage currents.
Guard rings are often employed to define a specific region in the detector that is sensitive to radiation.
Electrons and ions collected by the guard ring produce induced current that returns to ground without
adding to IRL = Vin . As a result, radiation interactions in the electric field region influenced by the guard
ring go undetected. The free air ion chamber, discussed in a later section, is one such example of an ion
chamber with a sensitive region well defined by a guard ring.
Sec. 9.5. Ion Chamber Designs 343

outer conductor inner


insulator
outer insulator
guard ring
inner insulator

center electrode
voltage i
supply current center
_ meter
+ electrode
gas-filled chamber virtual ground
Side View End View

Figure 9.26. Depiction of a coaxial ion chamber with a guard ring.

Coaxial Ion Chamber Designs


Coaxial detectors operate mainly with a positive voltage applied to the central electrode. For different
types of detectors, the anode diameter may range between 25 microns to a few hundred microns. Coaxial
proportional counters and coaxial Geiger-Müller counters typically have central anodes between 25 to 100
microns in diameter for reasons discussed in Chapters 10 and 11.
Due to the cylindrical geometry, there is a higher probability that gamma rays interact in the larger
volume of gas nearest the cathode than in the smaller volume near the anode. This effect is referred to
as geometrical weighting [McGregor and Rojeski 1999]. As a result the coaxial design reduces the position
dependence of the induced signal Vin that is transferred to the electronics, as shown in Fig. 9.22(a). Although
negative voltage can be applied to the anode, the average voltage signal produced is considerably less, as
shown in Fig. 9.22(b).
Guard rings are usually used in coaxial ion chambers as depicted in Fig. 9.26. Just as a guard ring is
used in a planar chamber, the guard ring is fashioned so that the leakage current is diverted from adding to
the detector signal. Detector leakage currents on the order of only 10−16 amp have been successfully realized
in designs of coaxial ion chambers. However, variations in the insulator design and other irregularities can
blur the edges of the active region in a coaxial ion chamber. Often a second guard ring is placed around
the first guard ring, referred to as a field tube, to define better the active region of the detector. Because
field tubes have a special importance to the operation of proportional counters, a discussion on field tubes
is delayed until Chapter 10.

9.5.2 Gamma-Ray Ion Chamber Designs


Gamma-ray ion chambers, operated in the current mode, are stable, have long lives, and they can be
fabricated in a variety of sizes and shapes. Large ion chambers are used as area monitors for ionizing radiation,
and high-pressure chambers offer a relatively high sensitivity, permitting measurement of exposure rates as
low as 1 μR/h. Small chambers with low gas pressures can be operated in radiation fields with exposure
rates as great as 107 R/h.
Because of the lower energy deposition (−dE/dx) of electrons compared to that of heavy charged particles,
electrons produced by gamma-ray interactions in the gas often have ranges greater than the dimensions of
an ion chamber. As a result, the energy deposition by electrons is usually less than that for heavy charged
particles and, consequently, the resulting input voltage Vin is smaller for electrons. Obviously, ion chambers
operating at relatively low gas pressures have lower efficiencies than those with higher pressures.
Sensitivity to gamma rays can be enhanced by lining the walls of the chambers with high Z materials to
increase the interaction probability. Recall from Chapter 3 that the total interaction coefficient for gamma
344 Gas-Filled Detectors: Ion Chambers Chap. 9

rays increases with the Z number. However, the electron range decreases with Z, thereby reducing the
sensitive wall thickness for which secondary electrons can escape into the detector gas.
Air-filled ionization chambers vented to atmospheric pressure are often used to measure radiation ex-
posure. After the formation of an electron-ion pair, the electrons and ions begin to move through the gas
towards their collecting electrodes. However, the electronegative oxygen atoms quickly capture free electrons
to produce heavy negative ions. Because of this electron attachment, most of the free electrons disappear and
the chamber current is produced by the motion of both negative and positive heavy ions. This condition is
not a problem when a detector is operated in the current mode as long as the potential difference is sufficient
to prevent significant charge recombination. However, such a chamber is not suited for pulse-mode operation,
because the positive and negative ions move slowly compared to electron speeds in the same electric field,
consequently, very few and indistinct pulses are produced.

9.5.3 Neutron-Sensitive Ion Chambers


If an ion chamber is coated with a neutron reactive material with a large neutron cross section or filled with
a neutron reactive gas, such that ionizing particles are released from the neutron reactions, the chamber can
be used as a neutron detector. Commonly used isotopes for neutron detectors are 3 He, 10 B, 6 Li, and 235 U.
Neutron sensitive ion chambers are usually filled with 10 BF3 or 3 He gas, or the inside walls of the chamber
are coated with 10 B, 6 LiF, or 235 U. These gas-filled neutron detectors can be operated as both ion chambers
or proportional counters.
Ion chambers that use 235 U are often referred to as fission chambers, since it is the fission fragments from
the 235 U that ionize the chamber gas. Fission chambers are often used in mixed radiation fields containing
large numbers of neutrons and gamma rays. Fission fragments deposit as much as 50 times the energy as
do gamma rays in a common fission chamber. Hence, when operated in pulse mode, the voltage pulses
formed by fission fragments are much larger than those formed by gamma rays, thereby making it possible
to discriminate between the two radiations. Due to pulse pile-up, ion and fission chambers are generally not
operated in pulse mode when in high radiation fields, although some special pulse mode designs incorporating
235
U are used for in-core nuclear reactor monitoring. Gas-filled neutron detectors are described with more
detail in Chapters 17 and 18.

9.5.4
a Compensated Ion Chambers
A form of ion chamber frequently used for control of nuclear
g-ray sensitive
chamber volume
Ig
- + reactors is known as the compensated ion chamber. Ion cham-
bers, when operated in current mode, can be used in high ra-
diation environments. If a gas-filled neutron detector is placed
central
electrode near a nuclear reactor, it responds to both neutrons and gamma
rays. Yet, current mode operation does not permit pulse-height
Ar gas discrimination between neutron and gamma ray interactions as
does pulse mode operation. The compensated ion chamber de-
In = Ig + n - Ig sign is used to distinguish between the two types of radiation in
10
high radiation fields.
B coating Typically the chamber has two concentric electrodes and a
neutron and g-ray central wire electrode. One concentric electrode is coated with
sensitive chamber volume Ig + n + - a neutron sensitive material such as 235 U or a compound con-
taining 10 B. The configuration depicted Fig. 9.27 allows both
Figure 9.27. Cross section diagram of a con-
centric compensated ion chamber.
chambers to experience the same radiation field. Differences be-
tween the two chambers can be properly calibrated by adjusting
Sec. 9.5. Ion Chamber Designs 345

the operating voltages. The 10 B (or 235 U) coated chamber is referred to as the working chamber and the
uncoated chamber is referred to as the compensating chamber. When exposed to both gamma rays and neu-
trons, the voltage potential for the working chamber causes current to flow that deflects the current meter
in one direction. The voltage potential in the compensating chamber, sensitive only to gamma rays, causes
current to flow in the opposite direction. The voltage potentials on the chambers can be adjusted such that
the two gamma ray signals exactly cancel. As a result, the compensated chamber produces a net current
that is directly proportional to the strength of the (thermal) neutron field. Compensated ion chambers are
widely used in nuclear reactors because of their ability to respond to neutron fields that vary up to ten orders
of magnitude; i.e., these detectors have a very large dynamic range.

9.5.5 Frisch Grid Ion Chambers


An ion chamber design attributed to Otto Frisch [Frisch 1942; Bunemann et al. 1949] practically eliminates
the dependence of the output pulse height on the position of the ionizing event in ion chambers, thereby
allowing the detector to be used as an energy spectrometer. Shown in Fig. 9.28 is the basic arrangement for a
Frisch grid or gridded ion chamber design. The gridded ion chamber is separated into two compartments: one
is a much larger main chamber and the other is the measurement or detector chamber. The two chambers
are separated by a conductive screen. Shielding can be arranged to confine radiation interactions to the
main chamber. A voltage is placed across both chambers by use of a resistive divider. The electric field is
applied such that the grid is positive with respect to the cathode, and the anode (the collecting electrode in
the measurement compartment) is positive with respect to the grid.
electrons that pass Gamma rays, or other ionizing particles,
into the measurement

Cm compartment produce Vin that interact in the main chamber produce


RL Vin(t)
Vm
t electron-ion pairs just as in any other ion
chamber. The positive ions drift toward the
shield td=dm /ve
dm cathode and electrons drift toward the grid.
- - However, the main chamber is not connected
grid - - incident te=(dch-x0) ions and electrons drifting
radiation ve in the main chamber do directly to the input, and the induced current
Vch dch not contribute to Vin
produced in the main chamber does not charge
+ +
+ +
x0 tion=x0 /vion the coupling capacitance. The grid essentially
0 Vin (t) shields the anode from induced current while
shield
charges move in the main chamber. As a
result, charges moving in the main chamber
compartment do not contribute to the voltage
Figure 9.28. Depiction of a Frisch grid ion chamber.
signal.
With sufficient speed, the electrons pass through the grid into the measurement compartment, which is
connected to the output electronics. As the electrons drift through the measurement compartment, they
induce an input voltage Vin (t)
qe N0 ve tm
Vin (t) = ,
dm

where tm is the drift time across the measurement compartment and dm is the length of the measurement
compartment. If there is no electron attachment, the input voltage reduces to qe N0 after all electrons
are collected. Note that the interaction position dependence has been eliminated from the input voltage.
Further, because positive ions do not contribute to the signal, the slow signal component usually observed
from ion drift is also eliminated, thereby reducing the effect of pulse height deficit.
346 Gas-Filled Detectors: Ion Chambers Chap. 9

9.5.6 Free Air Ion Chambers


A standard instrument used for radiation exposure measurements is the free air ion chamber. The traditional
radiation exposure unit, the Roentgen, abbreviated R, is defined precisely as the quantity of x or gamma
radiation that produces 2.58 × 10−4 coulomb of separated charge of either sign per kilogram of air in the
incremental volume where the primary photon interactions occur. The SI exposure unit, the X unit, equals
3881 R, which is defined as the amount of x or gamma radiation that produces 1 Coulomb of charge per kg
of air. Hence, by measuring the amount of ionization in air, the radiation exposure field can be determined.
This task can be accomplished with a free air ionization chamber.
The chamber is constructed as shown in
V sensitive Fig. 9.29 with one electrode is segmented to form
volume
a guard ring structure. The chamber is shielded
aperture with lead and is filled only with air at ambient
exit port
temperature. X or gamma rays enter through an
L
g rays aperture in the box, interact in the air, and whose
or
x-rays reaction products then ionize the air. However,
guard only the ionization formed in that region defined
guard wires
wires
by the radiation aperture and the center electrode
guard
(of width L) is measured, thereby giving an air
guard ring volume and the ionization. As a result, the radi-
ring electrode
electrode signal
ation exposure can be determined.
signal
collection to electrometer Here the initial assumption is that ion recom-
electrode
bination does not significantly affect measured re-
Figure 9.29. Free air ionization chamber configuration. sults. However, the high density of O2 indicates
that significant electron attachment will occur in
the chamber which can result in recombination losses. To reduce the effect of charge loss to recombination,
the ionized volume is kept small, and it is the replenishment of ionized charges in the sensitive volume that
indicates the radiation exposure.
Two important design features should be noted. First the interaction rate density along the photon
beam inside the chamber must be relatively constant, and second the length of the beam on either side of
the central portion of length L must be at least equal to the maximum distance in which ions are produced
from the primary photon interaction location. Thus, ions produced outside of L by interactions in L are
exactly compensated for by ions produced in L by photon interactions outside of L. This compensation is
called charged particle equilibrium [Shultis and Faw 2002] and is central to radiation dosimetry.
Because of the need for charge particle equilibrium, the use of the free air ionization chamber is limited
to photons with energies less than about 500 keV [Cember 1983]. Although larger units would allow mea-
surements of radiation exposure for higher energy gamma rays, such chambers appear to be impractically
large and would require much more extensive shielding.

Example 9.5: A free air ionization chamber is operated at 20◦ C with air pressure of 750 torr. The chamber
aperture diameter is 1 cm and the signal collection electrode is 4 cm in length. At 150 volts operating bias,
a current of 12 nA is measured. What is the radiation exposure rate?

Solution:
As discussed earlier, electron attachment is severe in air; hence, almost all electrons undergo electron
attachment before collection and, thereby produce heavy negative ions. However, because the exposed
volume is small compared to the chamber size, the positive and negative ions are quickly separated so that
it is assumed that few ions recombine.
Sec. 9.5. Ion Chamber Designs 347

The pressure and temperature must be corrected for the standard conditions of radiation exposure rate.
Hence,
dX I P0 T
=
dt ρ0 Vch P T0
where Vch is the sensitive volume of the chamber, ρ0 is the air density, and P0 and T0 are the standard
pressures (in torr) and absolute temperatures.
The sensitive volume is Vch = π(0.5)2 (4) cm3 = 3.14 cm3 . The density of air at standard conditions is
1.2922 × 10−6 kg/cm3 . The resulting exposure rate is
  
dX 1.2 × 10−8 A 760 torr 293.15 K
=
dt (1.2922 × 10−6 kg/cm3 )(3.14 cm3 ) 750 torr 273.15 K

= 3.214 × 10−3 X-units/sec = 12.47 R/sec

9.5.7 Pocket Ion Chambers


Compact ion chambers, often referred to as pocket ion chambers, are a convenient method to measure
exposure to radiation. There are fundamentally two types of pocket ion chambers, one is a condenser-type
chamber and the other an electroscope chamber, both shown in Fig. 9.30. The condenser-type ion chamber
is a form of air-wall ion chamber, in which the air volume is relatively small, usually on the order of 2 cm3 ,
with walls composed of “air-equivalent” material. The condenser pocket ion chamber operation is quite
simple. Coaxial in form, the outer portion is composed of electrically conducting plastic with a gamma-ray
response equivalent to pressurized air. A central wire is attached inside the chamber through insulating
standoffs, and is positively charged with respect to the outer wall. These chambers are typically backfilled
with air. As radiation interactions occur within the chamber walls, the resulting ionization discharges the
condenser such that the stored voltage decreases. The decrease in voltage is directly correlated to the energy
deposited within the chamber, thereby yielding a measure of the radiation exposure. The condenser pocket
ion chamber is conveniently simple, but must be read from a charging device. The sensitivity of common
condenser pocket ion chambers ranges from 25 mR to 250 R.
The electroscope pocket ion chamber is closely related to the gold leaf electroscope. These devices
are commonly used to measure relative radiation exposure for the wearer. The device consists of a tube
approximately 10 cm long and 1 cm in diameter. Inside the tube are two small metal-coated quartz fibers,
each approximately 4 microns in diameter. One of the quartz fibers is stationary and the other is hinged, and
both are inside an air cavity of the tube. The tube also has viewing optics such that when held up to a light,
the observer can see the shadow of the hinged quartz fiber against a display scale. The device is inserted into
a power supply and charged so that the two fibers, having like charges, are repulsed apart. This charged-up
device can now be worn as a dosimeter. Electrons produced by ionization caused by radiation interactions
in the chamber are attracted to the quartz fibers, thereby reducing the net charge and causing the quartz
fibers to move closer together. The change in location of the hinged fiber yields the change in exposure to
the wearer, which is determined by the change in location of the fiber with respect to the display scale in
the tube (maximum scale is usually 200 mR).14 The clear advantage of the electroscope pocket ion chamber
is the convenient method of viewing the exposure. However, interpretation of the exposure is visually left to
the user rather than a measuring instrument.

14 The Federal Civil Defense Administration (FCDA) had millions of pocket ion chambers produced during the 1950s and 1960s
for civilian use. By far the most popular pocket ion chamber, the V-742, was read in units of R with a maximum range of 200
R. Some of the units ranged up to 600 R (V-746), although the production run was limited to only a few hundred units.
348 Gas-Filled Detectors: Ion Chambers Chap. 9

anode insulator

charging
diaphragm

insulator conductive
plastic

metal coated
fiber metered
heavy quartz fiber
support lens scale lens
charging - - - - - - - - -
+ +
stem + +
+
+
eyepiece
+
+ +
window - - - - - - - - -

transparent metal coated


insulators movable quartz fiber

Figure 9.30. The basic components of a pocket ion chambers. (Top)


Depiction of a condenser-type pocket ion chamber. (Bottom) Depic-
tion of an electroscope pocket ion chamber.

9.5.8 Cloud Chambers


Cloud chambers are a type of ion chamber, but certainly not in the traditional electronic sense. Developed
by Charles Thomson Rees Wilson in 1911 (see [Wilson 1912]), the initial devices operated on the principle
of cooling by adiabatic expansion. In the original device, an ionizing radiation source was placed inside an
air-filled cylinder outfitted with a tightly sealed plunger. With the plunger in a nearly closed position, the
air in the cylinder compartment was saturated with water vapor. When the plunger is rapidly retracted, the
rapid decrease in temperature and pressure causes the water vapor to condense, particularly upon ions in the
chamber. The condensation upon these ions makes the ionization tracks visible to the eye. The effect is near
immediate and quite dramatic. Although the cloud chamber is a simple device, it led to numerous discoveries,
including the discovery of the positron (1932), the muon (1936), and the kaon (1947).15 The cloud chamber
works best with electro-negative gas molecules, for which electron attachment is rapid, thereby retarding the
diffusion of the negative ions and prolonging the visual effect [Sitar et al. 1993].

Expansion Cloud Chambers


Consider the expansion cloud chamber depicted in Fig. 9.31(a). The chamber is filled with a non-condensible
gas that adequately follows the ideal gas law. A vapor, water for instance, is added to the chamber such that
it reaches saturation. Initially, the partial pressure of the gas is Pg1 and the partial pressure of the vapor is
Pv1 . If the total mass of the vapor is mv1 at absolute temperature T1 and chamber volume V1 , then,
mv1
Pv1 V1 = RT1 (9.141)
M
where M is the molecular weight of the vapor molecules and R is a constant. If the piston is rapidly
retracted to cause a sudden expansion in the closed system, in which the volume V1 is expanded to V2 , then
the temperature immediately reduces from T1 to T2 . For an ideal gas, undergoing a reversible adiabatic

15 Forhis invention of the cloud chamber, Charles Thomson Rees Wilson shared the 1927 Nobel prize in physics with Arthur
Holly Compton.
Sec. 9.5. Ion Chamber Designs 349

camera

glass
window
light camera
source radiation
source
fill gas and glass
solvent vapor voltage window
glass solvent
cylinder reservoir
light
source radiation
solvent fill gas and source
solvent vapor
glass
container metal
piston
black plate
felt mat
piston base
cylinder dry ice

(a) (b)
Figure 9.31. (a) Basic components of an expansion cloud chamber and (b) basic components of
a diffusion cloud chamber.

process [Das Gupta and Ghosh 1946],


 γ−1
T1 V2
= , (9.142)
T2 V1
where γ is the adiabatic index16 for the gas mixture
CP
γ= . (9.143)
CV
Here CP is the specific heat capacity at constant pressure and CV is the specific heat capacity at constant
volume. Immediately after the expansion, but before condensation takes place, the new vapor partial pressure
is
mv1
P2 V2 = RT2 , (9.144)
M
where the vapor mass is the same as before, but now distributed over the new volume V2 . Yet, this state
is short lived, because the cooling causes part of the water vapor to condense, thereby changing the partial
pressure, vapor mass and the temperature (slightly). As equilibrium is reached, the temperature rises slightly
from T2 to T2 , caused by the condensation of vapor. The equilibrium condition is
mv2
P2 V2 = RT2 , (9.145)
M
where mv2 is the equilibrium vapor mass. The density of the vapor immediately after the piston is retracted
is represented by
mv1
ρ2 = (9.146)
V2
and after the system has reached equilibrium, the density of the vapor is
m2
ρ2 = . (9.147)
V2

16 Also called the heat capacity ratio or ratio of specific heats.


350 Gas-Filled Detectors: Ion Chambers Chap. 9

The amount of supersaturation can be defined as the ratio of the densities of ρ2 to ρ2 , i.e.,

ρ2 mv1 P1 V1 T2
S= = = . (9.148)
ρ2 mv2 P2 V2 T1

Dividing Eq. (9.144) by Eq. (9.145) also yields,

P2 T2
S= . (9.149)
P2 T2

If the temperature rise from condensation is small, then T2  T2 , and with the substitution of Eq. (9.142)
into Eq. (9.148) one obtains [Das Gupta and Ghosh 1946]
 γ  γ
P1 V1 P1 1
S = , (9.150)
P2 V2 P2 FC

where FC is the expansion ratio. Note that the supersaturation is strongly dependent upon γ and the partial
vapor pressure P2 . The required expansion ratio to produce a specific amount of supersaturation decreases
with increasing γ. Smaller expansion ratios are desirable because the lower amount of volumetric disturbance
reduces gas turbulence that can blur the ionization tracks.
The rapid decrease in gas temperature causes a supersatura-
tion of the water vapor, which enables the water to condense on
select surfaces. If the vapor pressure of small water droplets is
lower than the supersaturation, the droplets then grow in size,
and continue to increase in size until the vapor pressure of the
droplets corresponds to the supersaturation condition. As the
drops are forming, thermal conduction is heating the chamber
gas and reducing the degree of supersaturation, which rapidly
returns the gas mixture to the equilibrium condition. The time
duration over which the supersaturation conditions permit the
formation of visible tracks is relatively short, usually lasting
between a few milliseconds to a few seconds.
Viewing is best performed from the top of the chamber
through a clear glass window (see Fig. 9.31(a)). Gravity pulls
Figure 9.32. Ionization tracks produced by al-
the vapor tracks downward, and diffusion broadens the tracks.
pha particles in a cloud chamber [http://klarifi.
blogspot.com/search/label/nuclear Dec. 2013] Together these two effects serve to blur images if viewed from
the side; however, if viewed from the top, blurring from gravity
is kept to a minimum, as shown in Fig. 9.32. There is also the possibility of producing turbulence in the gas
when the piston is withdrawn, causing additional distortions in the ionization tracks.
Competing condensation surfaces include the chamber walls and foreign matter in the chamber. It can
be shown that small particle surfaces have higher vapor pressures than smooth planar surfaces [Staub 1953];
hence operating the system with optimized expansion ratios reduces (or eliminates) surface condensation
while permitting condensation on neutral and charged particles. The system can be cycled a few times to
reduce the background contamination, such as dust, from the system. Dust particles and other contaminants
appear as a faint fog in the chamber when first operated, but eventually drop into the solvent solution from
gravity, thereby being cleared from the gas after a few cycles. Tracks formed from ions can be cleared from
the system by temporarily applying a voltage across the chamber volume, which resets the system for the
next expansion operation.
Sec. 9.6. Summary 351

Diffusion Cloud Chambers


A simpler method of achieving the needed supersaturation condition is used in the diffusion cloud chamber
[Wilson 1951]. Depicted in Fig. 9.31(b), the diffusion cloud chamber operates with a temperature gradient
from the top to the bottom of the chamber. The chamber bottom is filled with dry ice and covered with a
metal plate. Typically a black felt or velvet mat is placed over the metal plate to improve viewing contrast.
A reservoir of solvent is placed near the top of the chamber. The entire chamber is covered with a transparent
window, usually glass, although modern cloud chambers have plastic lids. Often the lid is slightly warmed
to produce a thermal gradient from the lid to the chilled metal plate. The solvent vaporizes and diffuses
throughout the chamber, thereby causing the supersaturation condition to appear in the lower temperature
region of the chamber.
Diffusion cloud chambers are commonly operated with air as the gas and with either methanol or ethanol
as the solvent. These gases and vapors have good electron attachment, facilitating the formation of heavy
negative ions, which helps with the formation of visible particle tracks.
Advantages of the diffusion cloud chamber design include the continuous mode of operation and the lack
of moving parts, thereby reducing gas turbulence. However, the radiation source must be placed in a location
above the region of condensation or condensate coats the source and attenuates the ionizing radiation. For
alpha particle sources, the condensate can completely block the alpha particles from emerging into the
chamber. Because of its simplicity, diffusion cloud chambers are often used as demonstration devices for
classroom instruction.

9.5.9 Smoke Detector Ionization Chambers


A typical form of smoke detector commonly found in a household environment is actually a small free air
ionization chamber with an embedded 241 Am source that emits alpha particles. It can detect particles of
smoke that are too small to be visible. The alpha particles produce ionization in the tiny ion chamber, which
consists of an air-filled space between two electrodes, and permits a small, constant current to flow between
the electrodes. Smoke entering the chamber absorbs and neutralizes the alpha particles, thereby reducing
the alpha-particle induced ionization and current flow. This reduction in current sets off the alarm. Hot
air entering the chamber can change the rate of ionization, thereby altering the current and setting off the
alarm.

9.6 Summary
There are five distinct regions of operation for a gas-filled detector, the first two appearing at the lowest
voltages, identified as the recombination and ion chamber regions. At low applied voltages, charge pairs
may recombine, consequently nullifying, at least partially, the charge current induction effect necessary for
signal formation. The recombination probability is a strong function of the electron attachment coefficient,
the charge carrier diffusion coefficient, the gas density (pressure), and the applied voltage. At high enough
voltages, the free charges can be collected at the detector electrodes with reasonably high efficiency. Such
voltages are identified as the ionization chamber region of operation. Ion chambers can be operated in
current mode or pulse mode. Current mode operation is usually employed for relatively high radiation fields,
while pulse mode operation is usually employed for relatively low count rates (< 5 × 104 cps). Under pulse
mode operation, the signal from a ion chamber is strongly dependent on the electron motion and less so on
the heavy ion motion. Ion chambers can be acquired in a variety of configurations and are often application
specific.
352 Gas-Filled Detectors: Ion Chambers Chap. 9

PROBLEMS
1. A planar ion chamber with spacing between the electrodes of 3 cm is biased at 600 volts. The backfill
gas is P-10 filled at 1 atm. Unfortunately, the P-10 is contaminated with 0.04% O2 . Determine the
maximum fractional electron losses due to electron attachment for the detector.

2. Verify the general solution of Eqs. (9.79) and (9.80).

3. Use the boundary conditions to obtain solutions of Eqs. (9.81) and (9.82).

4. Verify the approximations of Eqs. (9.83) and (9.84), and then use these results to obtain Eqs. (9.85).

5. An ion chamber backfilled with air at 1 atm is operated at 200 volts. The electrode spacing is 4 cm.
The time constant of the detector is much less than the collection time for ions, but much longer than
the collection time for electrons. If a 5.5 MeV alpha particle enters into the chamber center parallel to
the electrodes and deposits all energy in the gas, what is the total value of free charge measured?

6. A planar ion chamber with electrodes spaced 2 cm apart is backfilled with 1 atm air at 20◦ C. Both
anode and cathode electrodes are square, with area 4 cm2 each. The chamber is then fully irradiated
with a one curie (Ci) 200-keV gamma-ray source at a distance of 25 cm from the detector. At what
voltage is the 90% saturation current reached?

7. Given the case in which ve vion , derive Eq. (9.126).

8. A free air ion chamber is operated at 200 volts.


The properties of the chamber include the following:
Electrode separation = 5 cm
Aperture diameter = 1.5 cm
Anode/cathode width = 2.5 cm
The operating conditions include:
Temperature = 82◦ F
Pressure = 1.05 atm
The operating response = 0.0095 μA
(a) What is the exposure rate from the radiation entering the chamber?
(b) The operator was in the radiation environment for 15 minutes. What is the integrated exposure in
X-units and roentgens?

9. The operating voltage of the free air ion chamber in Example 9.5 is increased to 200 volts with a resulting
current of 1.3 × 10−8 A. What is the corrected exposure as compared to the result of Example 9.5?

10. A pressurized condenser type pocket ion chamber has a chamber capacitance of 100 pF. When fully
charged, the chamber registers a voltage of 100 volts. The volume of the device is 10 cm3 , backfilled
with air at a pressure of 3 atm. After a tour of a radiation facility, the wearer of the ion chamber reads
a change in voltage of -4 volts. What was the radiation exposure?
References 353

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demic Press, 1966.
JAHNKE, E. AND F. EMDE, Tables of Functions with Formulae
BOAG, J.W., “Ionization Chambers,” Ch. 3, in Dosimetry of Ion- and Curves, New York: Dover, 1945.
izing Radiation, Vol. II, K.R. KASE, B. BJARNGARD, AND F.
ATTIX, eds., New York: Academic Press, 1986. KORFF, S.A., Electron and Nuclear Counters—Theory and Use,
New York: Van Nostrand Co., 1946.
BORTNER, T.E., G.S. HURST, AND W.G. STONE, “Drift Velocities
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Sci. Instrum., 28, 103–108, (1957). International Critical Tables of Numerical Data, Physics,
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Chapter 10

Gas-Filled Detectors:
Proportional Counters

I’ve worked on many detectors, some were very elegant and useless, and didn’t have a
Nobel Prize, so this one was not the most elegant, but it was useful.
Georges Charpak1

10.1 Introduction
ion pair recombination
Proportional counters are operated in region
occurs before collection III of the pulse height curve for gas detec-
Geiger-Muller
onset of region tors (see Fig. 10.1). In this region an elec-
“gas multiplication”
tronic pulse produced by ions moving through
transition the detector is proportional to the original en-
Pulse Height or Ions Collected

region
ergy absorbed in the detector gas by a radia-
tion particle, be they charged particles, neu-
trons, gamma rays or x rays. Although the
(log scale)

I II III gas-flow proportional counter was invented by


John A. Simpson, Jr., in the mid 1940s [Simp-
son 1950a, 1950b], the actual effect of pulse
a particles height proportionality was known from those
initial experiments conducted by Rutherford
IIIa IV V and Geiger with their gas-filled chambers. Ar-
gon is the most commonly used gas in a pro-
portional counter, although there are many
b particles other gases that can be used, such as 3 He, Xe,
and 10 BF3 .
Detector High Voltage (volts)
As with the ion chamber, a radiation par-
Figure 10.1. Proportional counters are operated in region III of the ticle can interact with the chamber, either di-
pulse height curve for gas-filled detectors. rectly with the chamber gas or with the cham-
ber walls. If a gamma ray interacts with the chamber wall and a primary or secondary energetic electron
escapes into the gas volume, this electron produces a cloud of electron-ion pairs. If the gamma ray inter-
acts directly with the gas, then the energetic electron produced by the interaction also produces a cloud
of electron-ion pairs. In either case, a cloud of electron-ion pairs is formed in which the total number of

1 Received the Nobel Prize in physics in 1992 for inventing the multiwire proportional counter.

355
356 Gas-Filled Detectors: Proportional Counters Chap. 10

electron-ion pairs produced is proportional to the radiation energy deposited in the detector gas. Hence,
by measuring the number of electron-ion pairs formed, the amount of energy deposited in the gas can be
determined. Application of a voltage across the chamber and measurement of the current produced as the
electrons and ions drift through the chamber volume allows the number of electron-ion pairs to be measured.
Yet, as with the ion chamber, such a current can be miniscule and hard to measure.

10.2 General Operation


ionizing
radiation
thin anode At sufficiently high voltages, electrons can gain enough ki-
wire
netic energy or speed to produce more ionization of the gas,
e- an effect called impact ionization. These newly liberated elec-
signal trons can themselves gain enough energy from the electric

high field field to cause even more ionization (depicted in Fig. 10.2).
region
e-
The process continues until the electrons are collected at the
anode. The entire process of generating the impact ioniza-
Townsend
avalanche ionizing tion cloud is called a Townsend avalanche, or sometimes gas
radiation V multiplication. There is a threshold electric field, Et , required
for avalanche multiplication, below which the electrons do not
Figure 10.2. With a high electric field near the
anode of a gas-filled detector, the signal is amplified gain sufficient energy to cause impact ionization. This thresh-
by impact or Townsend avalanching, often referred to old defines the difference between Region II and Region III
as “gas multiplication”. in the gas pulse height curve of Fig. 10.1.
Although parallel plate electrodes work for ion chambers, they are seldom used for proportional counters.
The preferred geometry is a coaxial configuration, as depicted in Fig. 10.3. To see why, compare the difference
in electric fields between coaxial and parallel plate geometries.
Gas Filled Regions
The parallel plate detector configuration is shown in Fig. 10.3.
A voltage Vo is applied to the electrode at x = x1 and zero
(grounded) at x = x2 . The electric field at any position between
the electrodes is
Vo Vo
a E(x) = = , (10.1)
b x 2 − x1 d
where d is the width between the parallel electrodes. Notice that
the electric field for a planar configuration is constant and, hence, a
x1 d x2
Planar Design Coaxial Design relatively large voltage is required to reach the threshold Et needed
(cross section)
to produce avalanching. By contrast consider the coaxial design
Figure 10.3. Planar and coaxial geometries shown in Fig. 10.3 in which a voltage Vo is applied to the inner
are often used for gas-filled radiation detec- anode and the outer electrode is grounded. The electric field at
tors. any radius r for a < r < b is, from Eq. (8.75),
Vo
E(r) = , (10.2)
r ln(b/a)
where a is the radius of the inner anode and b is the radius of the cathode shell wall. Unlike the planar case,
the electric field is not constant for the coaxial case, and the highest electric field is at r = a. Suppose the
distance between b and a in the cylindrical case is the same as the distance between x2 and x1 in the planar
case such that b − a = x2 − x1 = d. The condition is set such that the highest value of the electric field in
both cases just barely reaches the threshold electric field Et ,
Vo |cylindrical Vo |planar
Et = = . (10.3)
a ln(b/a) d
Sec. 10.3. Townsend Avalanche Multiplication 357

or
Vo |planar d
= , (10.4)
Vo |cylindrical a ln(b/a)
and, if a  b such that d = b − a ≈ b, then
Vo |planar b
≈ . (10.5)
Vo |cylindrical a ln(b/a)

Because a  b, b/a > 1 and the right-hand side of Eq. (10.5) is always greater than unity (usually 1).
Thus, for similar chamber dimensions it is found that the voltage needed to reach Et for the planar device is
always greater than that needed for the cylindrical device.

10.3 Townsend Avalanche Multiplication


At a threshold electric field Et electrons gain enough kinetic energy to produce impact ionization of neutral
gas atoms (or molecules). Although the exact value for Et varies with the gas, the threshold electric field
required for impact ionization is generally about 10 kV/cm. As the electric field is increased above Et , the
increase dn in the number of electron-ion pairs n(x) over a differential distance dx traveled by the electrons
is
dn = αT n(x)dx, (10.6)
where αT is the first Townsend ionization coefficient [Townsend 1915]. This coefficient can be interpreted as
the probability, per unit differential path length of travel, that an electron causes impact ionization.2 Also
the mean free path between impact ionization events is 1/αT .
From Eq. (10.6), the number of new electrons is found to increase exponentially with distance, i.e.,

n(x) = n(0) exp(αT x), (10.7)

where n(0) is the initial number of electron-ion pairs. The gas gain or gas multiplication M at distance x
from the initial location of the original electron-ion cloud is, therefore,
n(x)
M= = eαT x . (10.8)
n0
In Fig. 10.4 the first Townsend ionization coefficient is shown for various gases.
To achieve the necessary electric field threshold for a planar detector, potentials exceeding several thou-
sand volts must be applied across the electrodes. However, coaxial or hemispherical detectors can be operated
in region III of the gas pulse height curve with significantly lower voltages, commonly ranging between 200
and 1500 volts.
Consider a coaxial detector of radius b with anode wire of radius a, in which the electric field at the
surface of the anode is Et . Thus, from Eq. (10.2)
Vt
Et (a) ≈ 104 volts cm−1 = , (10.9)
a ln(b/a)
or the threshold voltage is approximately,
 
b
Vt = aEt ln ≈ 104 a ln(b/a) volts. (10.10)
a

2 Such a coefficient is analogous to the interaction coefficients for indirectly ionizing radiation discussed in Sec. 4.2.
358 Gas-Filled Detectors: Proportional Counters Chap. 10

 

 !"
 
 



    


      

 






 


 


 
 
         
            


Figure 10.4. The reduced first Townsend coefficient as a function of the reduced electric
field for several detector gases. From [Brown 1959].

The critical electric field needed for avalanching can be described in terms of the critical radius rc at the
onset of avalanche multiplication,
V0
Et = E(rc ) = . (10.11)
rc ln(b/a)
Equating Eq. (10.9) with Eq. (10.11) yields,
V0 rc
= . (10.12)
Vt a

Example 10.1: Consider a coaxial proportional counter backfilled with argon gas that is 1 inch in diameter
with a 25-micron diameter anode wire. Estimate the voltage required to reach the avalanche electric field at
the surface of the anode and compare the result to the expected voltage required for a planar detector with
a similar electrode spacing.

Solution:
From Eq. (10.9), the threshold voltage for the coaxial detector is,
 
(25 × 10−4 cm) (2)(2.54 cm)
Vt = (104 ) ln volts = 86.55 volts.
2 (2)(25 × 10−4 cm)
By comparison, a planar detector with electrode spacing of 1/2 inch would require
 
2.54 cm
Vt = (104 V/cm) = 12700 volts.
2

10.3.1 The Rose-Korff Formula for M


A commonly used, but simplistic, expression for the first Townsend coefficient can be derived by first con-
sidering the probability that an electron gains enough energy to produce impact ionization [Rice-Evans
Sec. 10.3. Townsend Avalanche Multiplication 359

1974]. Given an average distance Δx that an electron must traverse to gain enough energy to cause impact
ionization, the condition for impact ionization requires

qEΔx ≥ qI0 (10.13)

where E is the electric field and I0 is the ionization potential of the gas. The fraction of electrons with transit
paths ≥ Δx or, equivalently, have energies above Et needed to cause impact ionization is

ne (Δx)
= e−Δx/λ = e−I0 /λE , (10.14)
ne (0)

where ne (0) is the initial number of electrons produced from the radiation interaction event, and λ is electron
mean free path (for all types of interaction). The first Townsend coefficient is then the probability the electron
has E ≥ Et divided by the probability of an interaction in a unit differential distance of travel, namely3

ne (Δx) 1 1
αT = = e−I0 /λE . (10.15)
ne (0) λ λ

The mean free path λ is a function of the gas pressure and can be approximated by

1
λ= , (10.16)
AP

where A is an experimentally determined constant and P is the gas pressure. Substitution of Eq. (10.16)
into Eq. (10.15), the first Townsend coefficient is thus found to be [Korff 1946],

αT
= Ae−I0 AP/E = Ae−BP/E . (10.17)
P

For a limited range of the reduced electric field E/P , the microscopic cross section for impact ionization
σi is proportional to the electron energy Ee [Sauli 1977], i.e.,

σi = zEe , (10.18)

where z is an experimental constant. The mean free path between impact ionizations is

λi = 1/αT = 1/σi N (10.19)

where N is the atomic or molecular density of the chamber gas. Substitution of Eq. (10.18) into Eq. (10.19)
yields,
αT = zN Ee . (10.20)

Measured values for A, B, and z for several gases are listed in Table 10.1. From Eq. (10.17) it is seen that
αT increases as the electric field is raised above the avalanche threshold electric field Et .

3 Implicitin this derivation of αT is the assumption that, once E ≥ Et , the next interaction is an impact ionization event and
not, for example, a scatter.
360 Gas-Filled Detectors: Proportional Counters Chap. 10

Table 10.1. Some parameters used to calculate αT from Eq. (10.17), Eq. (10.18), and
Eq. (10.20). A and B are generally useful between 100 - 600 V cm−1 torr−1 , except H2
(150 - 600) and He (20 - 150). Data from [Brown 1959; Korff 1946; Rice-Evans 1974].

A B z
Gas
eip cm−1 torr−1 V cm−1 torr−1 1017 cm2 V−1

H2 5 130 0.46
He 3 34 0.11
N2 12 342 0.70
Ne 4 100 0.14
Ar 14 180 1.81

Multiplication in a Coaxial Detector If rc is the critical radius at which the electric field reaches the critical
electric field necessary for a Townsend avalanche to occur, then the total gain, or multiplication factor, is
given by  rc
M = exp αT (r)dr . (10.21)
a
The capacitance, per unit length, of a coaxial chamber is
2π0 κ
Cl = , (10.22)
ln(b/a)
where κ is the dielectric constant of the gas. Recall that the electric field depends upon the radius r, and
substitution of Eq. (10.22) into Eq. (10.2) gives this dependence as4
Vo Cl Vo
E(r) = = , (10.23)
r ln(b/a) 2πro κ
and
Vo ln(r/a) Cl Vo
V (r) = = ln(r/a). (10.24)
ln(b/a) 2πo κ
The average energy gained by electrons between impact ionizing collisions is, by definition,
E(r)
E e = λi E(r) = , (10.25)
αT
which, when substituted into Eq. (10.20), gives

αT = zN E(r). (10.26)
Substitution of Eq. (10.26) into Eq. (10.21) and use of Eq. (10.23) allows the gas multiplication to be
evaluated as
       
rc
Cl Vo Cl Vo 1/2 Cl Vo rc
M = exp zN dr = exp 2zN r −a 1/2
= exp 2azN −1 .
a 2πr0 κ π0 κ c π0 κ a
(10.27)

4 Notethat from Poisson’s equation, ∇2 V = −∇· E = −ρ/κ0 . Here the authors assume that the initial space charge is negligible
and use the magnitudes of the voltage and electric fields to determine M .
Sec. 10.3. Townsend Avalanche Multiplication 361

Table 10.2. The reduced first Townsend coefficient αT /P and the gas multiplication
factor M as a function of ln M/(aP Sa ) where Sa ≡ Ea /P . Here Sa ≡ S(a) and
Ea ≡ E(a). Also C1 to C14 , K1 to K10 , m, and d are empirical constants. The
formulas are from [Kowalski 1986].

Citation αT /P ln M/(aP Sa )
c1 √ c1
Rose and Korff [1941] S K1 − √
2 Sa
c2
Hristov [1957] c2 K1 −
Sa
Diethorn [1956] c3 S c3 (ln Sa − ln K3 )
 
−c5 c4 −c5
Townsend [1915] c4 exp (exp + K4 )
S c5 Sa
Williams, Sara [1962]
     
−c7 2c6 c7 −c7
Ward [1958] c6 exp √ K5 + √ + 1 exp √
S c27 Sa Sa
Charles [1972]
 
Sa c9
Zastawny [1966] c8 (S − S0 ) K6 + c 8 ln + −1
c9 Sa
c10 S 1.5 √
Kowalski [1985] c10 Sa + K7
2 
−c12 c11 1 m−1
Aoyama [1985] m
c11 S exp exp −c12 Sa + K8
S 1−m c12 1 − m
c13 d−1 c14
Kowalski [1986] c13 S d + c14 S − + K9
d−1 a Sa
c13
Kowalski [1986] c13 S d S d−1 + K10
d−1 a

Finally, substitution of Eq. (10.12) into Eq. (10.27) and use of Eq. (10.23) gives the following two equivalent
results

 * +
Cl Vo V0
M = exp 2azN −1
π0 κ Vt
 < * + . (10.28)
azN Vo V0
M = exp 2 −1
ln(b/a) Vt

Equation (10.28) represents the derived result of at least one formulation of the avalanche coefficient,
traditionally named the “Rose-Korff” formula [Rose and Korff 1941]. In the present case, Eq. (10.28) yields
acceptable results for many gases for which 10 ≤ M ≤ 103 [Staub 1953]. However, above this range, the
formulation of αT may need adjustment. Further, several experimental studies indicate that Eq. (10.28) has
limited use for many detector gas mixtures, and has limited use over a large range of gas detector design
parameters [Diethorn 1956; Kiser 1960; Zastawny 1966; Zastawny and Mizeraczyk, 1966]. Consequently,
there are many alternative empirical formulas for M listed in the literature [Kowalski 1986]. A summary of
these formulas is given in Table 10.2.
362 Gas-Filled Detectors: Proportional Counters Chap. 10

10.3.2 The Diethorn Formula for M


Another commonly used expression for M is the Diethorn formula [Diethorn 1956]. At a constant gas
pressure P in the detector chamber under a reduced electric field S(r) ≡ E(r)/P , the distance between
successive impact ionizations varies as 1/S. Also, within a constant reduced electric field S, the mean free
path between ionizing collisions varies with 1/P . Hence,
1 P 1
λi ∝ ∝ ∝ . (10.29)
SP EP E
This relation indicates that the distance between ionizing collisions decreases as the electric field increases
and is independent of the gas pressure P . The ionization mean free path λi can be much greater than the
collision mean free path λ. The kinetic energy acquired by an electron between successive ionizing events is,
qΔV = qλi E (10.30)
where ΔV is the potential difference that an electron must pass through over a distance λi in order to
obtain sufficiently kinetic energy to produce an ionizing event. From Eq. (10.29), ΔV must be a constant
characteristic of the fill gas. It is therefore assumed that the first Townsend coefficient is linearly related to
the electric field, or
αT E
=c , (10.31)
P P
where c is an experimentally determined constant. Also, for any gas pressure P , there is a critical threshold
electric field for the onset of avalanche multiplication, or
Et = KP, (10.32)
where K is an empirical constant.
Diethorn [1956] estimates the number of electron collisions producing secondary ionization as n = Vt /ΔV
where Vt is the potential at Et .5 Because the first ionization event yields 2 electrons both of which cause
subsequent ionization events, thereby doubling their number, and so on, then after n impact ionizations
there are 2n electrons for each initial electron. Thus, the multiplication factor is
Vt
M = 2n or ln M = n ln 2 = ln 2. (10.33)
ΔV
For a coaxial detector, the reduced electric field can be described by,
E(r) V0
S(r) = = . (10.34)
P rP ln(b/a)
with reduced potential distribution
V (r) V0 ln(r/a)
U (r) = = . (10.35)
P P ln(b/a)
Solve Eq. (10.34) for r and evaluate the result at the critical radius rc to obtain
V0
rc = (10.36)
b
Et ln
a
5 Diethorn’streatment indicates that a negative potential is applied to the cathode of a coaxial detector with the anode grounded,
a case rarely used, if ever. However, the treatment is mathematically correct. If instead a positive potential was applied to
the anode with the cathode grounded, the estimated number of ionizing collisions would be n = (V0 − Vt )/ΔV .
Sec. 10.3. Townsend Avalanche Multiplication 363

Table 10.3. Constants for different gases used to calculate M from Eq. (10.38).

ΔV K
Gas Citation
V V cm−1 torr−1

95% Xe/5% CO2 31.4 48.16 Hendricks [1972]


90% Xe/10% CH4 33.9 47.63 Hendricks [1972]
P-5 (95% Ar/5% CH4 ) 21.8 ± 4.4 59.21 ± 5.26 Wolff [1974]
P-10 (90% Ar/10% CH4 ) 23.6 ± 5.4 63.16 ± 3.95 Wolff [1974]
CH4 36.5 ± 5 90.79 ± 6.58 Wolff [1974]
C3 H 8 29.5 ± 2 131.58 ± 5.26 Wolff [1974]

Substitution of Eq. (10.32) and Eq. (10.36) into Eq. (10.35) yields,
⎛ ⎞
V0 ⎜ V0 ⎟
b ⎝ b⎠
Vt = ln . (10.37)
ln aKP ln
a a
Finally, substitution of Eq. (10.37) into Eq. (10.33) yields the Diethorn formula [Diethorn 1956],

 
V0 ln 2 V0
ln M = ln − ln K , (10.38)
ln(b/a) ΔV aP ln(b/a)

or the general form used in Table 10.2,

ln M ln 2
= (ln Sa − ln K) , (10.39)
aP Sa ΔV

where Sa ≡ S(a). Equation (10.38) is particularly useful for CH4 and many forms of Xe-CH4 and Ar-CH4
mixtures. Reported values for constants in Eq. (10.38) are listed in Table 10.3.

10.3.3 The Zastawny Formula for M


However, Eq. (10.38) is less useful for pure Ar, N2 , and CO2 , or for those gas mixtures involving CO2 . To
address the problems with Eq. (10.38), Zastawny [1966] developed an alternative solution to the Diethorn
equation (also listed in Table 10.2). Differentiation of Eq. (10.34) and evaluation of Sa = S(a) from this
equation gives the relation
aSa
dr = − 2 dS. (10.40)
S (r)
With this relation between dr and dS Eq. (10.21) may be expressed as
 Sa
αT (S) dS
ln M = aP Sa , (10.41)
S rc P S 2 (r)
364 Gas-Filled Detectors: Proportional Counters Chap. 10

Table 10.4. Constants for different gases used to calculate M from Eq. (10.43).

K c1 c2
Gas Citation
V−1 V1 V cm−1 torr1

CO2 0.5 × 10−3 1.93 × 10−2 69 Zastawny [1966]


N2 (0.655 ± 0.03) × 10−3 (18.6 ± 0.9) × 10−2 85 ± 4 Zastawny,
Mizeraczyk [1966]
Ar (6.25 ± 0.3) × 10−3 (39.6 ± 2) × 10−2 34 ± 2 Zastawny,
Mizeraczyk [1966]
P-10 (0.5 ± 0.1) × 10−3 (3.0 ± 0.03) × 10−2 25 ± 1 Zastawny [1967]
Xe/5% CO2 2.49 × 10−3 3.01 × 10−3 32.37 Hendricks [1972]
Xe/10% CH4 5.45 × 10−3 2.46 × 10−3 19.47 Hendricks [1972]

where Src = S(rc ) is the reduced electric field at the radial location for the onset of avalanching, and αT (S)
is the first Townsend coefficient as a function of the reduced electric field. Zastawny [1966] proposed
αT
= c1 (S − c2 ), (10.42)
P
which, when substituted into Eq. (10.41) yields,

 
ln M Sa c2
= K + c1 ln + −1 , (10.43)
aP Sa c2 Sa

where K, c1 , and c2 are experimentally determined constants. Experimental comparisons indicate that
Eq. (10.43) works well for Ar, N2 , CO2 , and mixtures of CO2 gas [Zastawny 1966, 1967; Zastawny and
Mizeraczyk 1966]. Reported values of constants in Eq. (10.43) for several gases are listed in Table 10.4.

10.3.4 The Kowalski Formula for M


Kowalski mentions that equations for M listed in Table 10.2 have diverse results when tested with various
gases over wide ranges of S. In an attempt to produce a generalized formula for the gas multiplication factor,
Kowalski suggests the use of
αT
= cS d (10.44)
P
where c and d are experimentally determined constants. Insertion of Eq. (10.44) into Eq. (10.41) yields

ln M c
= S d−1 + K (10.45)
aP Sa d−1 a

where K is an experimentally determined constant. When fit to data reported by various researchers,


Eq. (10.45) appears to have merit for a variety of complex gas mixtures, many of which are listed in Table 10.5.

10.4 Gas Dependence


The ionization potentials and electron mobilities for many detector gases are significantly different, many of
which are listed in Tables 9.1 and 9.2. The first Townsend coefficient should also vary among gases because
Sec. 10.4. Gas Dependence 365

Table 10.5. Constants for different gases used to calculate M from


Eq. (10.45). Data from [Kowalski 1986].

c K
Gas d
(mPa)d−1 V−d V−1

Ar 6.34 × 10−4 1.85 −6.79 × 10−3


Ar/5.7% C5 H12 1.46 × 10−3 1.775 −1.22 × 10−2
Ar/3.1% C5 H12 2.46 × 10−3 1.70 −1.52 × 10−2
Kr/4.11% C2 H6 O 2.14 × 10−3 1.525 −1.54 × 10−2
Kr/1.92% C2 H6 O 3.00 × 10−3 1.45 −1.97 × 10−2
Xe/6.16% H2 1.10 × 10−4 2.225 −3.02 × 10−3
Xe/16.7% Kr/7% H2 1.80 × 10−4 2.125 −4.08 × 10−3

M is strongly dependent on the mean free path length λi between ionizing collisions. As a result, gas
multiplication can vary significantly for different detector parameters, gases, and gas mixtures. Examples
of experimentally measured multiplication factors as a function of operating voltage are shown in Fig. 10.5
and Fig. 10.6.
Electron attachment, discussed in Sec. 9.2.5, can adversely affect the performance of proportional coun-
ters. Hence, gases with small electron attachment coefficients are commonly chosen as the gas in a propor-
tional counter and include CH4 , CO2 , and Ar. Extreme care is required to prevent contaminant gases with
relatively high electron attachment coefficients, such as O2 , from entering the detector.
Various gas mixtures are often introduced into the detector chamber to improve performance. Gas
additives and mixtures can improve electron velocities (see Fig. 9.6 and Fig. 9.7), improve avalanche gain,
decrease the required operating voltage, improve energy resolution, and eliminate spurious pulses. These gas
mixtures may include Penning mixtures to increase the number of charge carriers per ionizing event, and
may include quench gases to prevent successive avalanches from a single event.

10.4.1 Quenching Gas


After an impact collision, the resulting ion is often left in an excited state which can rapidly decay by
emitting a photon (usually in the ultraviolet). This photon may then interact photoelectrically with another
gas atom or molecule releasing a photoelectron which then causes another avalanche of electrons.
Let δ be the probability that an electron liberated through impact ionization leads to a tertiary electron
through photoionization (typically δ  1). The gas multiplication per initial electron-ion pair is then given
by

n
M = f + δf 2 + δ 2 f 3 + ... + δ n−1 f n = δ i−1 f i , (10.46)
i=1
where f is the total number of electrons liberated per primary electron-ion pair and would equal the multipli-
cation factor if there were no photoionization, i represents the consecutive avalanche number (first, second,
third, and so on) up to the final avalanche (n). Because δf is strongly dependent upon the applied operating
voltage and is generally less than unity, Eq. (10.46) reduces to
f
M= . (10.47)
1 − δf
If, in fact, δf > 1, the avalanching process becomes uncontrollable and the detector develops a self-
sustaining discharge, which may occur with too high of voltage (as in Region V). Continuous waves of
366 Gas-Filled Detectors: Proportional Counters Chap. 10

Figure 10.5. The multiplication factor M for Figure 10.6. The multiplication factor M for
several gases each at a pressure of 100 torr. The several gases and pressures. The detectors for
detectors for H2 , CH4 and Ar had a = 127μm and H2 (550 torr), CH4 (400 torr) and Ar (400 torr)
b = 11.05 mm. The BF3 detector had a = 127μm had a = 127μm and b = 11.05 mm. The BF3
and b = 19.05 mm. From [Staub 1953]. detector (804 torr) had a = 127μm and b = 19.05
mm. From [Staub 1953].

avalanches can occur if UV light released by excited ions causes photoionization of outer shell electrons in
too many more neutral Ar atoms. This is the most probable source of new electrons because of the high
opacity of the gas at UV energies. However, UV light striking the cathode may also release photoelectrons
from the cathode material. Finally, when a gas ion reaches the cathode wall, more electrons may be released
by two different mechanisms. First, the energy difference between the work function of the cathode material
and the ionization potential of the ion may be radiated into the tube gas as an ultraviolet photon which
may, in turn, interact with a gas atom releasing a photoelectron. Second, the energy difference may liberate
an electron directly from the cathode in a radiationless energy transfer. These mechanisms for starting
additional avalanches are depicted in Fig. 10.7(a).
To prevent continuous waves of avalanches from occurring in the chamber after a radiation interaction,
a small amount of a quenching gas is added to the gas mixture, typically a polyatomic molecule. When an
ionizing particle enters the detector, it ionizes both the host and the quenching gases. More important, the
argon ions, traveling towards the cathode, collide with a quenching gas molecules from which they readily
take an electron, thus transferring almost all of the positive charge to quench gas molecules. UV photons can
also interact with the quench gas, but the molecules dissociate instead of releasing photoelectrons. These
molecules, when reaching the cathode, dissociate rather than liberate electrons, as would an argon ion if it
were to strike the wall. In this manner further avalanches are suppressed. These quenching mechanisms are
depicted in Fig. 10.7(b).
Quench gases are usually chosen with ionization potentials below that of the host gas, a precaution that
allows charge to transfer from the host gas to the quench gas while rendering the reverse process improbable.
Sec. 10.4. Gas Dependence 367

excited
neutral
cathode molecule
wall

excited
UV photon neutral atom
emission

- photoelectron dissociation

cathode cathode
wall wall ionized
molecule

+ +
-
electron emission
dissociation

UV photon UV photon
+
photo-ionization

dissociation
-
(a) (b)
Figure 10.7. A quench gas is used to prevent continuous avalanches in the
proportional counter. When a noble gas ion or UV photon strikes the cathode
wall or a UV photon is absorbed by a neutral noble gas atom, electrons may
be ejected that can start another avalanche, as depicted in (a). The quench
gas, usually an organic molecule, dissociates when it strikes the cathode wall
or when it absorbs an energetic photon; hence it does not cause the release of
an electron that can start a new avalanche, as depicted in (b).

Quench gases should also not be electronegative so they are not prone to electron attachment. Several
different organic molecules have been successfully used as quench gases (see Table 10.6). As the host gas
ions drift through the chamber, they pass their charge to the quench gas molecules. These charged quench
gas ions continue to drift and carry the positive charge to the cathode wall. When a quench gas is either
struck by a UV photon or strikes the cathode wall, it dissociates, rather than eject an electron, as illustrated
in Fig. 10.7(b). As a result, the quench gas prevents continuous waves of ionization. A common proportional
counter gas mixture is P-10, which is a mixture of 90% Ar and 10% methane.

10.4.2 Penning Mixtures


Electron collisions in a gas can leave a gas in an excited state, which generally de-excites by the emission of
a photon. However, long-lived metastable states can also be formed by electron collisions, in which radiative
transitions to the ground state are forbidden. These excited metastable states do not produce ionization
and consequently do not add to the induced charge signal. However, if a small amount of gas is added to
the gas mixture, in which the added gas has a lower ionization potential than that of the excited metastable
state of the host gas, then the energy stored by the metastable state can be transferred through a collision
to produce another electron-ion pair,

A∗ + B → A + B + + e− , (10.48)
368 Gas-Filled Detectors: Proportional Counters Chap. 10

Table 10.6. Common detector host and quench gases with their ionization potentials
Io . From [Christophorou 1971].

Detector Gas Common Name Io (eV) Detector Gas Common Name Io (eV)

Ar Argon 15.755 CH4 Methane 12.98


He Helium 24.580 CO2 Carbon Dioxide 13.79
H2 Hydrogen 15.42 C2 H 2 Acetylene 11.36
O2 Oxygen 12.08 C2 H5 OH Ethyl Alcohol 10.50
N2 Nitrogen 15.6 C3 H 8 Propane 11.08
Ne Neon 21.559 C4 H10 Isobutane 10.55
Kr Krypton 13.996 Cl2 Chlorine 11.48
Xe Xenon 12.127 Br2 Bromine 10.55

known as the Penning effect [Penning 1927]. This gas additive is also referred to as a “quench gas”, although
the effect is quite different than described in the previous subsection. Quite instead, adding a Penning
quench gas increases ionization, and thereby increases the charge signal for the primary radiation absorption
event. In effect, the average ionization energy of the gas mixture is lower than either individual gas, which
works to improve charge collection statistics and improve energy resolution in a proportional counter [Sipilä
1976].
An example of the Penning effect is the small addition of Ar to a host gas of Ne. From Table 10.7, Ne
has a metastable state energy of 16.53 eV while Ar has a first ionization energy of 15.76 eV. Hence, the
metastable Ne gas atom can transfer sufficient energy to an Ar gas atom to produce an electron-ion pair.
Typically, excellent improvement is achieved with only 0.01% Ar added [Druyvesteyn and Penning 1940].
The Penning effect is also observed with numerous polyatomic gases, generally because polyatomic gases
have relatively low ionization energies (see Table 10.6). Experimental studies have shown that addition of
H2 C2 (acetylene) to the host gas Ar improves energy resolution for low avalanche gains (≤ 10) [Järvinen
and Sipilä 1984; Agrawal et al. 1989]. Studies with gas-filled proportional detectors have shown that ∼ 2%
Xe added to Ar does improve performance, providing higher avalanche gains than other mixtures tested in
the study [Agrawal et al. 1989], while a gas mixture of ∼ 20% Xe added to Ar produced improved energy
resolution (≈ 7% FWHM at 22 keV) nearly equal to mixtures of Ar/H2 C2 . In a similar study for multiple
organic gas additives with Xe as the host gas, a strong Penning effect was observed with trimethylamine
(Io ≈ 8.32 eV) and dimethylamine (Io ≈ 8.4 eV) as additives [Ramsey and Agrawal, 1989], where it is
reported that the Penning mixture of Ar + 5% trimethylamine allowed for a 50% reduction in operation
voltage while improving energy resolution by ≈ 22%.

10.5 Proportional Counter Operation


The creation of a pulse in a proportional counter starts with the initial ionizing event and ends with the
collection of the liberated charges at the electrodes (see Fig. 10.8). A radiation particle enters the detector,
interacts with the chamber gas, and liberates N0 electron-ion pairs. The electrons are quickly swept towards
the anode at speeds far exceeding those of the positive ions. Hence, the slow moving ions contribute very
little to the initial induced charge. Upon entering the avalanche region near the anode, the electrons create
numerous electron-ion pairs through impact ionization, equaling approximately N0 M , where M is the average
multiplication factor. The dense cloud of electrons is rapidly collected, leaving behind a dense cloud of slow
moving positive ions. These positive ions slowly drift towards the cathode. Because of the high weighting
potential in the anode region, it is the positive ions drifting from the anode towards the cathode that
contribute to nearly all of the input voltage Vin (t) to the amplification circuit.
Sec. 10.5. Proportional Counter Operation 369

Table 10.7. Ionization and excitation data for several gases. Data
from [Christophorou 1971; Rice-Evans 1974].

First Second First


Gas Ionization Ionization Excited Recombination
Energy Energy State Coefficient
(eV) (eV) (eV) (cm3 s−1 )

He 24.58 54.40 20.9 10−8


19.8 meta
Ne 21.559 41.07 16.68 2 × 10−7
16.53 meta
16.62 meta
Ar 15.755 27.52 11.56 9 × 10−7
11.49 meta
11.66 meta
Kr 13.996 24.56 9.98 10−5
9.86 meta
10.51 meta
Xe 12.127 21.2 8.39 2 × 10−6
8.28 meta
9.4 meta
H 13.60 10.2
N 14.53 29.59 6.3
O 13.61 35.11 9.1
H2 15.42 11.2 2 × 10−6
N2 15.6 6.1 2 × 10−6
O2 12.08 4 × 10−7
I2 9.0 1.9 1.5 × 10−8

10.5.1 Pulse Shape


The pulse shape of a coaxial gas-filled detector varies greatly depending on which region of the pulse height
gas curve of Fig. 10.1 the chamber is operated. The expected pulse shape for electron dominated voltage

cathode
+
+ + +
+ slow + + + +
+ moving ions + + + + + +
ions + + +
+ +
+ electrons ++ + +
+ + + + + Townsend +
+
+
anode ++ + + Avalanche +
++ ++ +
+ +
(a) (b) (c)

Figure 10.8. Pulse progression for a proportional counter: (a) an ionizing particle enters the
detector gas and creates electron-ion pairs, (b) the electrons rapidly drift towards the anode and
create an avalanche of electron-ion pairs, (c) the electrons are rapidly collected, whereas the positive
ions drift much more slowly towards the cathode. It is the positive ion drift that contributes to
most of the input pulse V (t) from a proportional counter.
370 Gas-Filled Detectors: Proportional Counters Chap. 10

pulses in a coaxial ion chamber was derived in Sec. 9.4.2. However, operating the same detector in the
proportional region causes a significant difference in the input pulse shape Vin (t). For simplicity, assume
that a radiation interaction creates a localized electron-ion cloud that can be treated as the location of N0
charged pairs at a single point. Initially, the input voltage induced by drifting electrons is essentially the same
as that in an ion chamber. However, once the electrons enter the avalanching region, a huge cloud of electron-
ion pairs is produced, mostly within a few microns of the anode. Because the total charge is increased by the
gas multiplication factor, most of the electron-ion pairs are produced very close to the anode. Consequently,
the drift distance for electron collection is relatively short, and the electron contribution to the input voltage
is relatively small. It is the motion of the cloud of positive ions drifting back towards the cathode that is
responsible for most the time-dependent input voltage. Hence, the input voltage in proportional counters is
positive ion dominated, whereas for ion chambers the input voltage is electron dominated.
Recall that the time dependent input pulse into the coupling electronics is

ΔQ(t)
Vin (t) = (10.49)
C
where C is the combined coupling and detector capacitance. The expression for ΔQ(t) for a coaxial detector
was derived in Sec. 8.7. Equation (8.80) with the variables used here is

ΔQ(t) = qN0 [ln(b/a)]−1 ln(rion (t)/re (t)). (10.50)

where rion (t) and re (t) are the radial locations of the positive ions and electrons, respectively, at time t.
Unlike an ion chamber in which only N0 electron-ion pairs are collected, in a proportional counter M N0
pairs are collected The electrons are rapidly collected in time te , leaving behind the positive ions to drift
toward the cathode. Almost all of the positive ions, save those very few produced in the original ionization
event, begin their drift, after all of the electrons are collected, essentially at the anode surface. Thus, for
t > te , Eq. (10.50) becomes

ΔQ(t) ≈ qM N0 ln(b/a)]−1 ln(rion (t)/a) t > te  0. (10.51)

The drift speed of the positive ions is given by

drion P0 μion E(r) P0 μion V0


vion ≡ = = . (10.52)
dt P rP ln(b/a)

The ion position rion (t) is found by integrating Eq. (10.52) as


 r(t)  t 2
P0 μion V0 rion a2 P0 μion V0
r dr = dt or − = t.
a P ln(b/a) 0 2 2 P ln(b/a)

Rearrangement of this last result yields


<
2P0 μion V0 t
rion (t) = + a2 . (10.53)
P ln(b/a)

Upon substitution of Eq. (10.53) into Eq. (10.50) and use of Eq. (10.49) the input voltage is
*< +
qM N0 2P0 μion V0 t
Vin (t) ≈ ln +1 , te < t < tion , (10.54)
C ln(b/a) a2 P ln(b/a)
Sec. 10.5. Proportional Counter Operation 371

for which the collection time for the positive ions is 


(b − a )P ln(b/a)
2 2


tion = . (10.55) 
2P0 μion V0
 
The maximum input voltage Vmax is found by eval- 

 

uating Eq. (10.54) at t = tion . The normalized input  
voltage V (t)/Vmax is, thus 
*< + 


Vin (t) 1 2P0 μion V0 t
≈ ln + 1 . (10.56) 
Vmax ln(b/a) a2 P ln(b/a) 


The magnitude of V (t)/Vmax initially rises rapidly, a           

fortuitous characteristic of the coaxial detector design,      

and is due to the combined effects of an initially high Figure 10.9. The normalized time-dependent input volt-
positive ion speed because of the high electric field near age V (t)/Vmax for a proportional counter as a function
the anode and the enhanced weighting potential near of t/tion for different values of Rba = b/a as given by
the anode. For example, the time required to reach Eq. (10.56). For the results shown, b = 1.25 cm and
a = b/Rba .
half the maximum input voltage Vmax /2 is found from
Eq. (10.56) as
b a2 P ln(b/a)
tVmax /2 = −1 . (10.57)
a 2P0 μion V0
The normalized time-dependent input voltages V (t)/Vmax as a function of t/tion are shown in Fig. 10.9 for
different values of Rba ≡ b/a.

Example 10.2: A coaxial proportional counter backfilled with argon at 1 atm is operated at 1000 volts.
The detector has an anode radius of a = 25 microns and cathode radius b = 1.25 cm. Exclude the possibility
of a time delay caused by space charge. At what time past t = 0 does the input voltage V (t) reach 1/2 the
maximum possible pulse height? How far have the positive ions drifted in the chamber?

Solution:
From Table 9.2, the mobility μ+ 2
ion at 1 atm for argon is 1.7 cm V
−1 −1
s . The ratio b/a = 500. The
maximum speed of the positive ions is found from Eq. (10.52) as

P0 μion V0 (1 atm)(1.7 cm2 V−1 s−1 )(1000 V)


vmax = = = 0.109 cm/μs.
aP ln(b/a) (25 ×−4 cm)(1 atm) ln(500)
The highest positive-ion speed is less than the saturation speed shown in Fig. 9.6, thereby validating the use
of the ion-speed approximation. From Eq. (10.57)

b a2 P ln(b/a) (25 ×−4 cm)2 (1 atm) ln(500)


tVmax /2 = −1 = [500 − 1] = 5.7 × 10−6 seconds.
a 2P0 μion V0 2(1 atm)(1.7 cm2 V−1 s−1 )1000 V
Insertion of this result into Eq. (10.53), the radial location is
<
2P0 μion V0 t
r(tVmax /2 ) = + a2
P ln(b/a)
<
2(1 atm)(1.7 cm2 V−1 s−1 )(1000 V)(5.7 × 10−6 s)
= + (25 ×−4 cm)2 = 0.0559 cm = 559 μm,
(1 atm) ln(500)
372 Gas-Filled Detectors: Proportional Counters Chap. 10

which indicates that the positive ions have drifted

d = (559 − 25) μm = 534 μm.

The input voltage Vin (t) from a proportional counter is often applied to a preamplifier CR-RC circuit
(as is done with an ion chamber). From Eqs. (9.118) and (10.56), the output voltage of the preamplifier is
τo
Vout (t) = Vin (t) e−t/τo − e−t/τi ,
τo − τi
*< +
qM N0 2P0 μion V0 t τo
= ln +1 e−t/τo − e−t/τi . (10.58)
C ln(b/a) a2 P ln(b/a) τo − τi

With the same analysis used to obtain Eq. (9.120) for the case τo = τi , Eq. (10.58) reduces to
*< +
qM N0 2P0 μion V0 t t −t/τ
Vout (t) = ln 2
+1 e . (10.59)
C ln(b/a) a P ln(b/a) τ

Typically the time constant of the circuit


is adjusted to be much shorter than the to-
tal time required to collect the positive ions;
otherwise, the recovery time would result in
significant dead time loss. However, because
a large portion of the input voltage is induced
within the first several microseconds, the time
constant can be adjusted to be small while
still allowing the induction of large input cur-
rents. For monoenergetic events, the propor-
tional counter nearly eliminates the position
dependent charge collection issues typical of
ion chambers. In principle, proportional coun-
ters should be capable of operating as energy
spectrometers provided there is strict propor-
tionality, i.e., M does not depend on the pri-
Figure 10.10. Electron drift speeds, measured at room temperature mary ionization. This requirement is true if
(293–300 K), for several detector gases as a function of reduced elec- space-charge effects by the positive ions are
tric field. Data from [Bowe 1960; Brown 1959; Cottrell and Walker negligible (see Sec. 10.5.2) and if all the elec-
1965; Pack and Phelps 1961; Phelps et al. 1960].
trons have approximately the same travel dis-
tance and produce the same avalanche multiplication. This last requirement is achieved by using a very thin
anode wire, typically a few hundred μm in radius. Thus, the high electric fields that cause avalanching are
very close to the anode and almost all secondary ionization is in a very small volume around the anode.
Radiation interactions rarely create electron-ion pairs at a point location. Typically, radiation charged
particles or charged particle reaction products have paths oriented over all possible directions in the cham-
ber. The situation is further complicated for energetic electrons because they move along very tortuous
trajectories (see Fig. 4.22). For instance, a cloud of electron-ion pairs oriented parallel to the central anode
wire produces a time-dependent input pulse similar to that described by Eq. (10.54). However, an ion pair
Sec. 10.5. Proportional Counter Operation 373

track perpendicular to the anode wire produces an input voltage distorted from those shown in Fig. 10.9.
Those electrons liberated nearest the anode start an avalanche at time t0 , whereas those electrons liberated
furthest from the anode enter the avalanche region at t0 + Δt, where Δt is the time required for all the
electrons to drift into the avalanche region. As a result, the rise of Vin (t) is further extended over Δt causing
a distortion in the shape of the input voltage. Consequently, the input pulses can have different maxima
for monoenergetic events, thereby compromising the energy resolution of the proportional counter. This
problem of varying pulse heights, with examples, is discussed in the literature [Gott and Charles 1969]. To
reduce the effect, it is typical to choose proportional gases with high electron mobilities and low electron
attachment coefficients. Recall from Chapter 9 that electron drift speeds in Ar are relatively low. The same
is true for other noble gases such as Kr and Xe. However, the average electron speed can be significantly
increased by adding small portions of CH4 or CO2 into the proportional gas (for example, compare Fig. 9.6
and Fig. 9.7). Shown in Fig. 10.10 are the speed characteristics as a function of reduced electric field for
several gases often used in proportional counters.

10.5.2 Space Charge Effects


As detailed by Wilkinson [1950] space charge accumulation can affect the gain, and ultimately the energy
resolution, of a proportional counter. The buildup of space charge has two basic formation mechanisms,
namely, self-induced space charge and cumulative space charge [Hendricks 1969; Mori and Watanabe 1982].
Self-induced space charge appears as an accumulation of positive charge near the anode as a consequence
of the avalanching process. This buildup of positive charge around the anode decreases the electric field in
the region nearest the anode wire. This space charge causes the local avalanche region around the anode
to decrease in size and causes a slight decrease in gain. The higher the radiation energy deposited in the
chamber, or rather, the more initial electron-ion pairs produced, the more avalanche electron-ion pairs are
produced. Hence, the space charge effect can introduce a small amount of non-proportionality in the detector
response at moderate operating voltages. As the operating voltage is increased, the multiplication factor
increases (see Fig. 10.5 and Fig. 10.6) and a larger cloud of space charge is formed. Hence, increasing the
operating voltage also increases the non-proportionality response to energy deposition and, generally, causes
a decrease in the expected pulse height [Fergason 1966]. Eventually, at sufficiently high voltages, the detector
is driven into the transition region (region IIIa of Fig. 10.1), in which pulses have limited proportionality to
the energy deposited in the detector chamber.
Cumulative space charge appears as a consequence of multiple events contributing to the total number
of drifting positive ions. Recall that, for those positive ions originating near the anode, the drifting times
required to reach the cathode can be relatively long compared to the electron drift time. During that drifting
period of the ions, additional radiation interaction events may occur that create additional clouds of positive
ions near the anode and which drift, in sequence, towards the cathode. Although these ions are drifting in a
region of low electrical field, the cumulative effect of multiple ion cloud formations causes the total electric
field to drop, including that in the avalanching region. Consequently, the induced charge is observed to
decrease from that expected from a single event [Burkhalter 1966]. This space charge effect becomes worse
with higher count rate, in which the uncertainty in pulse height for monoenergetic radiations increases, and
the average spectral shift in pulse height increases [Hendricks 1969]. To reduce the overall effect of space
charge within the chamber, it has been recommended that the gas gain M be kept low [Wilkinson 1950;
Hendricks 1969].

10.5.3 Counting Curve


It is always a good practice to calibrate gas-filled detectors before conducting measurements. For survey
instruments, such a calibration may be performed once per year with sufficient confidence in the measurement
374 Gas-Filled Detectors: Proportional Counters Chap. 10

results. However, laboratory instrumentation coupled to modular counting equipment, such as NIM or
CAMAC, requires calibration much more often. The reason why, of course, is because of the possible
frequent changes in equipment settings made by other users, such as the amplifier gain or the lower level
discriminator (LLD) setting, changes which alter the overall detector response. Consequently, before any
radiation measurements are conducted, a counting curve is usually first created to locate region III of the
pulse height curve for the chamber being used and also for the type of radiation particle being measured in
the samples.
Ideally, one should use a known source that emits the energy and type of particle to be measured in
the samples. For example, suppose the samples were thought to contain a radionuclide that emits an alpha
particle of energy Eo . Then with a check source that emits the same alpha particle energy, the lower level
discriminator (LLD) is adjusted by observing, with an oscilloscope, the amplitudes of the pulses being sent
to the counter. The LLD is set to reject pulses produced by background and other lower amplitude pulses
produced by other radiations. In this fashion only the higher amplitude pulses formed by the alpha particle
of energy Eo are counted.
Once the LLD is set, a series of measurements or
Table 10.8. Data for the counting curve of Fig. 10.11. counts of the radiation source are recorded at incre-
HV Counts HV Counts HV Counts HV Counts mentally increasing voltages beginning with a very low
or zero voltage. Each measurement has the same time
0 0 250 560 500 658 750 711 duration. As the output pulses triggered by the radia-
25 0 275 620 525 692 775 707 tion sources become larger, a direct result of increasing
50 0 300 645 550 698 800 725
75 0 325 669 575 654 825 720
M with applied voltage, they eventually pass through
100 10 350 642 600 693 850 754 the LLD and are counted. The counts for each mea-
125 23 375 659 625 703 875 832 surement are plotted versus the operating voltage used.
150 37 400 685 650 667 900 900 For a monoenergetic α particle source, as the operat-
175 65 425 648 675 686 925 1130
ing voltage is increased, eventually almost every out-
200 123 450 671 700 714 950 1342
225 349 475 667 727 683 975 1800 put pulse from the radiation source exceeds the LLD,
and the number of counts per measurement reaches a
near constant value over a finite voltage region as shown in Fig. 10.11. As the voltage is increased further,
the avalanche gain in the chamber continues to increase until eventually lower energy radiations from the
source or background radiations create pulses that also pass through the LLD, at which point the count rate
rapidly increases. Usually, the operator selects an operating voltage in the center of the perceived counting
plateau to conduct the sample measurements.
A measure of the performance of a proportional counter is the slope of counting plateau. To obtain the
slope first draw a smooth line through the data points and, somewhat subjectively, determine the voltage
Va at the start of the plateau and the voltage Vb and the end of the plateau. The fractional plateau slope is
given by
  
Ctsb − Ctsa 2
slope = (10.60)
Vb − Va Ctsb + Ctsa

where Ctsa and Ctsb are the measured counts at operating voltages Va and Vb , respectively.6

6 An alternative expression is
  
Ctsb − Ctsa 1
slope = ,
Vb − Va Ctsa
where ΔCts is divided by Ctsa . But, because proportional counters are operated in the counting plateau center, and because
of the subjective nature of choosing the counting plateau limits, the authors believe that dividing by the average counts offers
a better representation of the fractional slope.
Sec. 10.5. Proportional Counter Operation 375




    
!" # $%%&      
   

  "'   
 ( #   
)" $%%&

 

         
  

Figure 10.11. A counting curve for a gas-filled proportional counter in which a mo-
noenergetic alpha particle source was used to calibrate the detector counting plateau.

The slope can also be expressed in terms of percent change per 100 volts of operating potential,
  
100(Ctsb − Ctsa ) 2
% slope|100V = 100 . (10.61)
Vb − Va Ctsb + Ctsa

Example 10.3: Measurements were conducted with a proportional counter with a monoenergetic α-
particle source for many operating voltages and yielded the data of Table 10.8. These data were used to
construct Fig. 10.11. Determine the % slope of the detector.

Solution:
The limits of the counting plateau are determined to be Va = 350 volts and Vb = 675 volts, yielding
  
cntsb − cntsa 2
slope =
Vb − Va cntsb + cntsa
  
686 cnts − 642 cnts 2
= = 0.000204
675 volts − 350 volts 686 cnts + 642 cnts

  
100(cntsb − cntsa ) 2
% slope|100V = 100
Vb − Va cntsb + cntsa
= 2.04% per 100 volts.

Source and Detector Effects


Quite often a source may emit several different radiations. Such mixed sources may emit alpha particles,
beta particles and gamma-rays of different energies. If performed correctly, the proportional counting can be
used to distinguish among the different radiations and their energies. Consider the pulse height histogram
of Fig. 10.12, showing the spectral features of a mixed source that emits alpha and beta particles.
376 Gas-Filled Detectors: Proportional Counters Chap. 10

a1 a2
dN plateau

Counts
background &
dE
electronic noise b
b plateau
a1
plateau
a2

E V
Figure 10.12. Depiction of the differential pulse height spectrum from a mixed α and β
particle source and the resulting counting curve for a relatively large volume proportional
counter.

For many proportional counter designs, the ranges of the α or β particles are longer than the chamber
dimensions. In other words, the particles do not deposit all of their initial energy in the detector. Because
the differential energy deposition, or stopping power −dE/dx, is much greater for α particles than that for β
particles, the density of the ionized charge cloud produced by the α particles is greater than that produced
by β particles. Consequently, the operating voltage required to produce pulses exceeding the LLD is lower
for α particles than β particles.
As shown in Fig. 10.12, the highest energy α particle yields a counting plateau at the lowest operating
voltage. The α particle with the lower energy, α1 , requires a higher operating voltage to produce a counting
plateau. Note that the counting plateau for α1 includes the sum of counts from both α2 and α1 . At a higher
voltage, the β particle source produces its counting plateau.
Because β particles are emitted with a continuum of energies, ranging from zero to Emax , the counting
plateau for β particles has a much higher increasing slope with increasing operating voltage than do the
slopes for the alpha particles. Consider Fig. 10.12, in which a beta particle spectrum is depicted. As the
operating voltage increases, the highest energy β particles eventually are able to produce pulses above the
LLD. As the operating voltage is increased further, more β particles with lower energies produce pulses above
the LLD, a trend that continues with increasing voltage. At high enough voltages, background counts are
included in the measurements, as well as the possibility of including spurious “counts” from the high electric
field, thereby causing a rapid increase in counts unrelated to the radiation source.
Electrons ejected by γ-ray interactions, β particles and positrons all have similar stopping powers −dE/dx
in the detector gas. Usually, proportional counter chambers are not large enough to capture all of the energy
from β particle emissions before they collide with the chamber wall. Consequently, the counting plateau
usually appears at a similar location in the counting curve regardless of the energy of the electron. Distinction
among energies becomes difficult unless the detector chamber is large enough to absorb all (or most) of the
energy. However, such chambers are very much larger than normal proportional counters. Note that large
gas-filled chambers do exist, many used for high energy physics experiments that require the capture of all
or much of the energy from weakly ionizing particles.
For some proportional counters, particularly pancake designs, the chamber dimension parallel with the
particle trajectories can be so small that higher energy α particles lose less energy in the chamber than
lower energy α particles, thereby producing less ionization than the lower energy α particles; hence, the
appearance of the counting plateaus is reversed in order from that normally expected. The case becomes
clear by considering the Bragg ionization curves depicted in Fig. 10.13. In this case the highest energy α
particles deposit the least amount of energy before striking the chamber wall. As a result, it is the lowest
Sec. 10.5. Proportional Counter Operation 377

detector
chamber
a3

Counts
plateau
a2 a3
plateau
a2
plateau
a1
detector
window a1

Figure 10.13. Depiction of Bragg ionization curves for multiple α particle energies as they
intersect a narrow detector chamber and the resulting counting curve. The shaded regions in
the Bragg ionization curves depict the integrated energy deposited in the chamber.

energy α particle that produces a counting plateau at the lowest operating voltage. Example radioactive
sources that can exhibit this property with pancake proportional counters include 228 Th and 226 Ra. Note
that particles entering the detector at oblique angles deposit more energy in the detector; however, the flat
portion of the counting plateau appears when nearly all particles of a particular energy produce pulses above
the LLD. Under appropriate detector design and operating conditions, it is possible that the different alpha
particles have overlapping counting plateaus, making distinction among them difficult.

10.5.4 Fluctuations of the Gas Multiplication Process


Because the proportional counter maintains a proportional relation between absorbed energy and the input
pulse Vin (t), it is possible to operate proportional counters as energy spectrometers. Consider the case of a
monoenergetic radiation source, in which the emitted radiations deposit their total energy into the detector
upon each interaction. The average number of secondary electrons m produced through avalanching by a
single initial electron is given by a PDF paval (m) with a mean m and a variance σ 2 (m). Various models
for paval (m) are presented later in this section.
For a single event that produces n initial electron-ion pairs, there is an average multiplication factor
M (n) for the total avalanche shower, that is given by


n
M (n)  mi , (10.62)
i=1

where the {mi } are random variables sampled from paval (m) representing independent electron avalanches.
The average multiplication per initial electron is

1
n
1
m= mi = M (n), (10.63)
n i=1 n

whose variance is
1  2
n
σ 2 (m)
σ 2 (m) = σ (m i ) = . (10.64)
n2 i=1 n
378 Gas-Filled Detectors: Proportional Counters Chap. 10

The expected or mean value of M (n), a sum of n independent random variables (the {mi }), is

@
n
A n
M  = mi = mi  = nm, (10.65)
i=1 i=1

and the variance is [Dunn and Shultis 2012]



n 
n 
n
σ 2 (M ) = σ 2 mi + 2 covar(mi , mj ). (10.66)
i=1 i=1 j=1
j<i

If the {mi } are independent and identically distributed,7 then the covariances vanish leaving

n 
n
σ 2 (M ) = σ 2 mi = σ 2 (m) = nσ 2 (m). (10.67)
i=1 i=1

For a given source, detector, geometry, etc., the probability that a radiation event produced n electron-
ion pairs in the chamber gas is denoted by pin (n) with a mean n and variance σ 2 (n). This PDF is very
complex because it involves modeling the electron-ion pairs produced along the trajectory of the incident
radiation particle. As a result no explicit expression for pin (n) is usually available, but, conceptually, it
exists.
A pulse height spectrum is a histogram depicting the frequency of observing the total charge Q liberated
in a detector. For each monoenergetic radiation particle interacting within the detector, there are nj electron-
ion pairs initially liberated, and the shower produced has an average multiplication factor mj . As information
is accumulated, i.e., more interaction events are observed, an average number of initial electron-ion pairs
n becomes evident as does an average multiplication factor M . The average charge collected over multiple
monoenergetic events is, therefore, Q = qnM where


nM  nM  = ni M (ni )pin (ni ). (10.68)
i=1

The variance σ 2 (Q) defines the theoretical limit on energy resolution for a proportional counter. Two
sources of variance are identified above, namely, the variance σ 2 (n) in the initial number of electron-ion
pairs produced and the variance σ 2 (m) in the multiplication factor for each avalanche triggered by an initial
electron. Because n and m are independent variables, simple error propagation can be used to give
 2  2
σ 2 (Q) σ(n) σ(m)
2 = + . (10.69)
Q n m

Substitution of Eq. (10.64) into Eq. (10.69) yields


 2  2
σ 2 (Q) σ(n) 1 σ(m)
2 = + . (10.70)
Q n n m

For a purely stochastic Poisson process, the expected variance for n is σ 2 (n) = n, where n = E/w, E is
the energy deposited in the detector and w is the average ionization energy. Therefore, the expected standard

7 This assumption is not valid if the positive ions create significant space-charge effects.
Sec. 10.5. Proportional Counter Operation 379

error for a Poisson distribution is σ(n) = E/w. However, Fano [1947] points out that the ionization process
does not strictly follow a Poisson probability density function.
The process by which charged particles lose energy by impacting gas atoms to produce electron-ion pairs
is complex. One can measure the distance in the gas that an alpha particle travels (Δx) and the associated
energy loss (−ΔEα ). After numerous trials, fluctuations are observed in ΔEα about some average value
ΔEα . Now consider the inverse case, in which the change in energy ΔEα is constant and the associated
fluctuation in Δx is recorded. Such a problem is similar to the alpha particle straggling issue described in
Chapter 4.
Suppose it is determined that the average energy lost over distance x0 is E0 . If instead, the alpha particle
loses energy E over distance x0 , then it is expected that the average energy loss E0 is achieved within an
additional travel distance Δx, such that
x0 (E0 − E)
Δx = . (10.71)
E0
Note that Δx may be positive or negative. For any amount of energy lost, there is an average number of
electron-ion pairs w produced for that energy loss, thereby producing an average number of ions n0 for a
defined energy loss E0 . If, instead, the alpha particle produces n ionizations along Δx while losing the energy
E, then it is expected that the difference in ionization is realized within,
(E0 − E)
Δn = . (10.72)
w
Adding n to both sides of this result and using E0 /w = n0 one obtains
E
n + Δn − n0 = n − . (10.73)
w
Consider a charged particle that has a total of I ionization Table 10.9. Fano factors for several detector
impacts with the host gas. For the ith impact, ni is the number gases.
of ionizations produced and ui is the energy lost. The result of Gas F Citation
each impact is independent of other impacts; hence, averaged
over many histories it can be assumed that ni = n for all ni , He 0.20 Alkhazov 1969
Ne 0.13 Grosswendt 1984
and ui = u for all ui . It is therefore shown, for distance x0 , Ar 0.17 Alkhazov 1967
I = E0 /u = n0 /n, and the variance is [Fano 1947] Kr 0.19 Krajcar-Bronić 1998
Xe 0.18–0.32 Dias 1997
σn2 0 = (n − E/w)2  = I(ni − ui /w)2  = F n0 , (10.74) CO2 0.32 Alkhazov 1967
CH4 0.26 Alkhazov 1967
where F is C2 H 2 0.27 Alkhazov 1967
(ni − ui /w)2 
F = , (10.75)
n
and is traditionally called the Fano factor. The Fano factor accounts for the deviation from statistical
fluctuations expected with a Poisson distribution. Hence, the Fano factor can be defined as
observed variance
F = . (10.76)
expected variance from Poisson statistics
Equation (10.70) then can be rewritten as,
 2
σ 2 (Q) F 1 σ(m)
2 = + . (10.77)
Q n n m
380 Gas-Filled Detectors: Proportional Counters Chap. 10

Experimental measurements and theoretical calculations of Fano factors for various gases and gas mixtures
have been reported in the literature with varying agreement [for example, Alkhazov et al. 1967, Alkhazov
and Vorobe’ev 1969; Grosswendt 1984; Dias et al. 1997; Pansky et al.1997; Krajcar-Bronić 1998]. Dias et
al. [1997] and Pansky et al. [1997] report that the Fano factor is dependent upon the initial energy of the
primary ionizing particle, particularly important near photon absorption edges. The Fano factors for several
gases are given in Table 10.9.
The Avalanche Distribution Function paval (m)
The theory of electron multiplication seeks to find the probability distribution function paval (m) that gives
the probability that an avalanche initiated by a single electron produces m electrons. This distribution
problem has been studied by Snyder [1947], Frisch [1947, 1959], and Wijsman [1949]. All make several
simplifying assumptions. Secondary electrons are produced only by impact ionization (one per impact) and
production by photoionization is neglected. Recombination, electron attachment, and space charge effects
are likewise neglected. Finally, the probability of an impact ionization is solely dependent upon the electron
distance from surface of the anode.
In this section the approach used by Wijsman [1949] to find paval for a planar device is followed, In
such a device, avalanching can occur anywhere within the chamber, i.e., avalanching could occur anywhere
between the cathode (x = 0) and the anode (x = d). In Wijsman’s approach it is also assumed that an
impact collision creates only one additional electron.
Consider a coaxial ion chamber with the central wire as the anode. As electrons approach the inner anode
wire, the avalanche region begins at the critical radius rc from the coaxial center. When electrons enter the
region defined by radius rc , they attain sufficient kinetic energy to cause impact ionization. A local radial
coordinate x is now introduced such that x = 0 at rc and x = 1 at anode radius a, i.e.,
rc − r
x= , a ≤ r ≤ rc . (10.78)
rc − a

The probability an electron causes an ionization within dx about x is αT (x)dx, where αT is the first
Townsend coefficient. Wijsman sought p(n, x) the probability that a single electron that started at x = 0
had grown to an avalanche of n electrons at a distance x. The probability no ionization occurs between
x = 0 and x is  x
p(1, x) = exp[−τ (x)], where τ (x) = αT (x ) dx . (10.79)
0

To find p(n, x), proceed as follows. The probability the avalanche contains n − 1 electrons at x is
p(n − 1, x ). The probability that one and only one of these electrons causes an ionization between x and
x + dx is the probability that one of the (n − 1) electrons causes an ionization multiplied by the probability
that the other (n − 2) electrons produce no ionization, i.e., (n − 1)αT (x )dx [1 − αT (x )dx ]n−2 . As dx → 0
this probability becomes,
(n − 1)αT (x )dx . (10.80)
Now the avalanche contains n electrons and the probability that none causes further ionizations between x
and x is
exp[−n{τ (x) − τ (x )}]. (10.81)
To find p(n, x) multiply p(n − 1, x ) by the factors of Eqs. (10.80) and (10.81) and integrate over (0, x) to
obtain, for n > 1,
 x
p(n, x) = p(n − 1, x )(n − 1)αT (x ) exp[−n{τ (x) − τ (x )}]dx . (10.82)
0
Sec. 10.5. Proportional Counter Operation 381

To solve this equation for p(n, x), subject to Eq. (10.79), use a change of variables y(x) = exp[τ (x)] from
which it is found y(0) = 1 and dy/y = dτ . Let q(n, y) ≡ y n p(n, y). Equation (10.82) transforms to
 y
q(n, y) = (n − 1) q(n − 1, y  ) dy  . (10.83)
1

Differentiation of this equation gives


dq(n, y)
= (n − 1)q(n − 1, y) with q(1, y) = 1. (10.84)
dy
Solve these equations successively by induction for n = 2, 3, 4, . . . to find

q(n, y) = (y − 1)n−1 . (10.85)

Finally, transforming y back to x, the solution of Eq. (10.82) is

p(n, x) = exp[−nτ (x)]{exp[τ (x)] − 1}n−1 . (10.86)

In particular, when the avalanche reaches the anode, x = 1 and n → m so

p(m, 1) = exp[−mτ (1)]{exp[τ (1)] − 1}m−1 , (10.87)

or in terms of the original coordinate system

p(m, a) = exp[−mτ (a)]{exp[τ (a)] − 1}m−1 , (10.88)

where the “optical thickness” of the avalanche region is


 rc
τ (a) = αT (r ) dr . (10.89)
a

This distribution is known as the Furry distribution.8 It is easily shown




m ≡ m = mp(m, a) = exp[τ (a)]. (10.90)
m=1

Thus, paval (m|m) is given by


 m−1
1 1
paval (m|m) = 1− . (10.91)
m m

8 Thisdistribution was derived earlier by Furry [1937] who was studying electron showers produced by very high energy electrons
incident on lead. Furry found the number n of secondary electrons produced in a lead sheet of thickness t was given by
p(n|λt) = e−λt (1 − e−λt )n−1 , n ≥ 1,
where λ is an interaction coefficient with units of reciprocal length. The mean of this PDF is n = eλt so the PDF can be
written as  
1 1 n−1
p(n|t) = 1− .
n n
It is interesting that two different problems yield the same result. Wijsman was unaware of this earlier work, but because of
Furry’s primacy, the distribution of Eq. (10.91) is named after him.
382 Gas-Filled Detectors: Proportional Counters Chap. 10

The second moment of this PDF is m2  = 2m2 − m, so the relative variance is
σ 2 (m) 1
2 =1− . (10.92)
m m
For large values of m, which is usually the case, Eq. (10.92) reduces to [Lansiart and Morucci 1962],
σ 2 (m)
= 1. (10.93)
m2
Equation (10.91) can be expanded as
  2  3 
1 1 1 2 1 1
paval (m|m) = 1 − (m − 1) + (m − 3m + 2) −O . (10.94)
m m 2 m m

In the limit of large m


1 m 1 m 2 1 m
paval (m|m)  1− +  exp − . (10.95)
m m 2 m m m

For values of m > 9


∼ 50, Eq. (10.95) approximates Eq. (10.91) quite well. It should be noted that this
exponential PDF gives large fluctuations in m about the mean. Genz [1973] also points out that, for low
values of the reduced electric field (E/P ), the exponential approximation of the Furry model of Eq. (10.95)
adequately describes the probability distribution of avalanche electrons.
Effects of High Electric Fields
However, as noted by Byrne [1962], the Furry model fails to predict the observed results reported for
the distribution function of m under high electric field conditions [Curran et al. 1949]. The Furry model
was initially developed for high-speed particle impacts and it was assumed that the electrons have equal
probability of the causing impact ionization, within a differential distance of travel, regardless of their origin.
Thus, the effects of high electric fields, which accelerate the electrons, were ignored. In a coaxial gas detector,
as the electron shower progresses, the distance between ionizing collisions decreases because of the increasing
electric field as electrons approach the anode. Further, as the applied electric field is increased, eventually
the average distance between collisions in the highest field region is about the same as the minimum travel
distance for impact ionization, thereby fluctuations about m are suppressed [Schlumbohm 1958a]. As a
result, it is not surprising the Furry model does not hold for high values of E/P .
Distribution functions paval (m) from avalanche data for different values of E/P are given in the literature
for selected gases [Curran 1949; Schlumbohm 1958a, 1958b; Cookson and Lewis 1966a, 1966b; Genz 1973].
From the literature, it becomes apparent that at high values of E/P the data distribution functions deviate
from the exponential approximation of the Furry PDF but, instead, develop a maxima in the distribution
as can be seen in Fig. 10.14. Several alternative models have been proposed to account for the high-field
measured distributions of paval (m). These models are discussed by Genz [1973], and are shown to match
the measured distributions with varying degrees of success. One of the more popular models is based on the
Pólya statistical model [Pólya 1930]. Arley [1943] introduced the use of the Pólya model for the analysis of
an electron shower in lead, a similar problem considered by Furry.

9 From Eq. (10.95) the relative variance is found to be,


 ∞
1 m
σ2 (m) = (m − m)2 exp − dm = m2 ,
0 m m
so that σ2 (m)/m2 = 1, in agreement with Eq. (10.93).
Sec. 10.5. Proportional Counter Operation 383

Figure 10.14. Measured multiplication factor distributions for methane gas at reduced electric
fields of (a) 48, (b) 120, (c) 156, and (d) 218 V cm−1 torr−1 . Only under the lowest electric field
reported (a) does the distribution follow Furry’s prediction. The other distributions shown in (b)–(d)
resemble a Pólya distribution. Data from [Cookson and Lewis 1966b].

Byrne [1962] relaxed many of the assumptions used by Wijsman and developed a more general expression
for paval (m). In the present notation, Byrne obtained
 m
m (1)(1 + b)...(1 + (m − 1)b)
paval (m|m) = (1 + bm)−1/b , m ≥ 1. (10.96)
1 + bm m!
This PDF is the Pólya distribution, also known more commonly as the negative binomial distribution, in
which b ≥ 0 is a parameter.
The first and second moments of Eq. (10.96) are [Byrne 1962],

m = m and m2  = (1 + b)m2 + m. (10.97)

Hence, σ 2 (m) = m2  − m2 = bm2 + m and the relative variance is thus

σ 2 (m) 1
=b+ . (10.98)
(m)2 m

Some measurements of the relative variance indicate that average values as low as 0.45 can be expected
[Sipila 1976]. For large values of m, the limiting case for Eq. (10.98) reduces to,

σ 2 (m)
= b, (10.99)
(m)2
384 Gas-Filled Detectors: Proportional Counters Chap. 10



    



   
 

   
 

 






       



Figure 10.15. The Pólya distributions of (Eq. (10.102)) for m = 100 and
θ = 0, 0.1, 0.5, 1.0, 1.5, 2.0, and 2.5.

a result reported by Lansiart and Morucci [1962].


Cookson and Lewis [1966a] assumed that the first Townsend coefficient αT can be represented as
 
θ
αT = αT (max) 1 + , (10.100)
m
where αT (max) is the limiting value of αT for large m (m >∼ 100) and θ ≥ 0 is a parameter dependent upon
the gas type and operating conditions. Byrne [1962] and Cookson and Lewis [1966b] demonstrated that the
assumption of Eq. (10.100) leads to a Pólya distribution,
* +?b−1 * +
?b 1 ?bm ?bm
paval (m|m) = exp − , (10.101)
m (?b − 1)! m m

where ?b = b−1 = (θ + 1) and ?b ≥ 1. Byrne showed that as ?b increases above unity (or θ increases above zero),
Eq. (10.101) has a maximum at increasing values of m, as shown in Fig. 10.15. The physical significance
of θ (or ?b) is debatable. Byrne [1962, 1969] suggests that it represents the fraction of electrons above the
necessary gas ionization energy in the presence of large numbers of electrons. However, Cookson and Lewis
[1966a] and Alkhazov [1970] have contested Byrne’s explanation of θ (and ?b). Limiting conditions indicate
that for ?b → 1 (or θ → 0), Eq. (10.102) reduces to the Furry statistical model, whereas when ?b → ∞,
Eq. (10.102) reduces to the Poisson statistical model.
With a value of ?b  3/2, Eq. (10.101) agreed with the measured values of Curran et al. [1949]. This
agreement supports the validity of using the Pólya model for the electron avalanche. Substitution of ?b =
(1 + θ) into Eq. (10.101) yields,

 θ  
(1 + θ) 1 (1 + θ)m (1 + θ)m
paval (m|m) = exp − . (10.102)
Γ(1 + θ) m m m
Sec. 10.5. Proportional Counter Operation 385

The total limiting variance for the avalanche electron population is found by substituting Eq. (10.92) or
Eq. (10.98) into Eq. (10.77), thereby yielding
 
σ 2 (Q) F 1 1
2 = + 1− , (10.103)
Q n n m

for low E/P values, and


 
σ 2 (Q) F 1 1 1
= + + , (10.104)
Q
2 n n ?b m

for high E/P values.

Example 10.4: Determine the limiting resolution for 122-keV γ rays in a proportional counter backfilled
with Ar for which m = 100. Disregard any recombination effects.

Solution:
From Table 10.9, F = 0.17 for Ar, and from Table 9.1, w = 26 eV/iep pair for Ar. Assume a value of
b ≈ 0.45. From Eq. (10.104) and use of n = Eγ /w
   
σ 2 (Q) w 1 1 26 eV/eip pair 1
= F + + = 0.17 + 0.45 + = 1.34 × 10−4 .
Q
2
Eγ ?b M 122000 eV 100

The fractional energy resolution is defined as,


 
FWHM √ σ(Q)
= 2 2 ln 2 = 0.0273. (10.105)
Q Q

This result predicts an energy resolution of 2.73%.

In practice, the energy resolution of a proportional counter of the magnitude predicted by Example 10.4
is unusually small because many other factors affect the energy resolution. Sources of resolution degradation
include noisy electronics, varying gas pressure, gas impurities, avalanche saturation, anode wire eccentricity
and end effects, and anode wire uniformity [Charles and Cooke 1968].
Sources of electronic noise include variations in operating voltages from the high voltage power supply,
detector leakage current and amplifier electronic noise, all of which can be reduced to negligible levels for
well-designed equipment. Gas pressure variations can be caused by temperature changes, or, for gas-flow
systems, by variations in the gas flow, although such variations are usually small if the measurement period
is relatively short. Gas impurities can alter ion speeds and increase electron attachment. However, if the gas
detector system is thoroughly purged with a purified counting gas before use, the effect of gas impurities on
energy resolution can be eliminated. The gas flushing should be conducted long enough to remove moisture
contamination from the system interior surfaces.
Avalanche saturation causes the appearance of non-linear pulse heights, a result of operating the counter
in Region IIIa, the transition region, as was discussed in Sec. 10.5.2. To reduce the shift in pulse heights,
Spielberg [1967] reports that larger diameter wires produce less signal variance, and that tungsten wires
show smaller shifts in pulse heights than do steel wires. Limiting counting rates below 2000 cps also helps
minimize the variance [Charles and Cooke 1968]. Anode wire eccentricity can create axial non-uniformities in
the electric field, thereby adding to the variance about m, although this effect is generally small in well-built
386 Gas-Filled Detectors: Proportional Counters Chap. 10

proportional counters [Rossi and Staub, 1949]. The uniformity of the wire has been shown also to affect the
shift in pulse heights [Spielberg 1967], but thermal cleaning (heating to temperatures capable of evaporating a
microscopic layer from the wire) improved performance. However, the benefit of thermally cleaning degraded
over a period of a week, presumably from deposition of gas products upon the wires. Indeed, for proportional
counters in a high radiation environment, the breakdown of counting gases, especially those with organic
quenching gases, tends to coat the anode wires and leads to an increase in electrical resistance and wire
diameter. As a result, the variance in the avalanching electric field increases the variance about m. Despite
these complications, energy resolutions below 8% FWHM have been reported for low-energy gamma rays
[Charles and Cooke 1968, Sakurai and Ramsey 1992], and below 2% FWHM for neutron induced reaction
products [Oed 1988].

10.6 Selected Proportional Counter Variations


Since their introduction by Geiger and Rutherford in 1908, gas-filled detectors have been used widely for
many different radiation measurements, ranging from small pocket dosimeters to large chambers for high-
energy physics measurements. Proportional counters are of particular interest, mainly due to their high signal
gain while preserving energy deposition information. There are two basic types of proportional counters: gas
flow detectors and sealed detectors. Proportional counters can detect charged particles, energetic photons,
and neutrons. They are made in many sizes and shapes, too many to describe in this chapter, although many
variations are described elsewhere [Rossi and Staub 1949; Staub 1953; Price 1964; Sauli 2014]. However,
some common proportional counter geometries, along with a few uniquely interesting detectors, are described
in the following sections.

10.6.1 Gas-Flow Proportional Counters


Gas flow detectors are operated with the detection gas being constantly replenished during operation. This
constant gas replenishment allows gas molecules degraded from ionizing interactions to be removed and
replaced with fresh gas molecules. Moreover, the gas supply can be shut off when not in operation. Gas flow
detectors can operate indefinitely, provided that a gas source is available. Consequently, gas flow detectors
are usually operated as laboratory instruments due to the inconvenient requirement of an external gas supply.
This requirement makes portable instrumentation awkward.

2π and 4π Counters
The general construction of a 2π proportional counter is depicted in Fig. 10.16. The chamber is usually
cylindrical, as shown in Fig. 10.17; but sometimes the chamber may be hemispherical. In either case,
a radioactive sample placed in the chamber, usually through a rotating sample changer, is exposed to a
detector solid angle of 2π steradians; hence the name “2π counter”. An anode wire loop extends into the
chamber through an insulating high-voltage electrical feedthrough. Typically, the anode wire is on the order
of 25 to 75 microns in diameter, often composed of a gold-tungsten alloy. For safety reasons, positive high
voltage is applied to the anode wire while casing of the chamber is kept at ground potential.
The usual gas used in a gas-flow counter is P-10, and flows into the chamber through an input port and
exits through a gas metering device, such as a “bubbler” or gas flow meter. A common flow rate is “one
bubble per second”, which is about 50 to 60 sccm (standard cubic cm per minute). Because a detector
remains unvented between uses, it is common practice to purge the detector with the chosen detection gas
for several minutes before operation, usually at a higher flow rate than used during operation. For instance,
the purge may use gas flows >300 sccm to remove any air from the chamber, but then is reduced to about
55 sccm during operation. The reduction in gas flow reduces the possibility of perturbing charge collection
in the chamber, with the added advantage of conserving the detector gas.
Sec. 10.6. Selected Proportional Counter Variations 387

connector

anode
out
gas
chamber
bubbler source

in

source holder baseplate Figure 10.17. A 2π gas-flow pro-


portional counter, showing the de-
Figure 10.16. Diagram of a 2π gas-flow proportional tector base-plate, bubbler, 2π de-
counter. tector, and gas inlet.

A major feature of the “windowless” gas flow detector depicted in Fig. 10.16 and Fig. 10.17 is the absence
of an attenuating medium between the radiation source and the detector, because the source is inside the
detector. In the 2π detector approximately 50% of emissions enter the detector gas, although self-absorption
and backscattering effects must still be taken into account. Alpha particles, with ranges of a few centimeters,
deposit a large fraction of their energy in the chamber. Beta particles, usually having ranges up to tens
of centimeters, usually deposit only a small portion of their energy in the chamber. Gamma rays usually
interact in the walls of a proportional counter rather than with the gas. Interactions in the wall can eject
energetic electrons into the gas chamber. The stopping power −dE/dx is much higher for alpha particles than
for beta particles (or electrons/positrons). As a result, for sources that emit both alpha and beta particles,
a counting curve similar to that shown in Fig. 10.12 is expected, in which the alpha particle plateau(s)
appears at a much lower voltage than the beta particle plateau. Consequently, beta particles and gamma
rays are easily discriminated against by setting the high voltage to the center of the alpha particle counting
plateau and adjusting the LLD above the pulse heights produced by beta particles and gamma rays. The
windowless gas-flow detector also has the advantage of being able to detect low energy beta particles that
would otherwise be attenuated by the intervening air and the detector window. This advantage is important
for radionuclides that emit low energy beta particle such as 14 C and 3 H, provided that such sources are
properly prepared so as to reduce self-absorption effects.10
The 4π windowless gas-flow detector is designed so the radioactive source is placed upon a thin platform
between two 2π detectors [Martin and Green 1958]. If the combined thickness of the platform and radioactive
sample is relatively thin compared to the ranges of the particles of interest, then almost all of emitted particles
enter one of the detector halves. This configuration reduces uncertainty from backscattering, although self-
absorption may still be an issue. These devices have been used to measure absolute beta particle activities.
For radiation particles ejected simultaneously in relatively opposite directions, the two halves of a 4π counter
can be operated in coincidence to record only those events (or operated in anti-coincidence to reject those
events).

Thin Window Counters


Gas-flow detectors with thin windows are used when the radioactive source is outside of the detector, thereby
restricting the detector solid angle to <2π. A common laboratory thin-window gas-flow detector configuration

10 Low energy beta particles are more commonly measured with liquid scintillation detectors, covered in Chapter 13.
388 Gas-Filled Detectors: Proportional Counters Chap. 10

out connector in

anode

gas
chamber

thin source
window holder
source

Figure 10.18. Diagram of a thin-window, gas-flow, Figure 10.19. A thin-window,


proportional counter. A multi-wire anode is depicted in gas-flow, proportional counter,
the figure; however, many thin-film proportional coun- showing a metallized boPET win-
ters have a single wire loop for the anode. dow and sample holder slots.

is shown schematically in Fig. 10.18 and a photograph is given in Fig. 10.19. Commercial units commonly
have windows fabricated from thin boPET material that has been aluminized to block interference from
electromagnetic and visible light. The windows typically have mass thicknesses of about 0.4 to 2.0 mg/cm2 .
To avoid damaging the window, the gas exit port must remain unobstructed.11 Gas purge and operational
flow rates are similar to those used for windowless gas-flow detectors.
Disadvantages of using a thin-window gas-flow proportional detector include decreased detector solid
angle, parallax effects (see Sec. 7.5), and particle backscattering off the window. However, thin-window
chambers are usually compact and relatively easy to load. Unlike windowless gas-flow detectors, the radioac-
tive source distance for many thin-window detectors is variable, either incrementally with shelving slots,
as shown in Fig. 10.18 and Fig. 10.19, or with the source mounted on a retractable threaded rod. Some
commercial proportional counters have a head that can be mounted to a customized measurement system.
Thin-window gas-flow detectors, used as portable units at frisking stations, can have windows ranging
from 25 to 100 cm2 window area. They also have input ports for constant gas replenishment as shown in
Fig. 10.20. Some commercial models have the gas input through the detector cable rather than through a
separate gas supply line, thus simplifying cable/detector connections. The gas exits the detector through a
pin-sized hole located at the top of the detector body. Thin-window gas-flow detectors are also configured
as floor monitors, in which the detector height with respect to the floor is adjustable. The systems include
a gas supply bottle, portable cart, readout ratemeter, and cable connections.
Specially designed thin-window, gas-flow, proportional counters are used for detection of low energy
photons, such as characteristic x-rays [Goldstein et al. 1981], and are often used in measurement systems
for wavelength dispersive x ray spectroscopy. The windows of these detectors can be made from boPET;
however, higher transmission for low energies is obtained with lower density windows, such as polypropylene
(1 to 6-microns thick) and Formvar R
(polyvinyl formal), usually < 1 micron thick. For example, a 6 micron
thick boPET window absorbs 74% Al-Kα (1.487 keV), 85% Mg-Kα (1.254 keV), 92% Na-Kα (1.041 keV)
and 99% F-Kα (0.677 keV) x rays (see Fig. 10.22). Overall, polypropylene of the same thickness (6 microns)
absorbs approximately 60% fewer low energy photons than does boPET, consequently, it is routinely used
for detection of characteristic x rays emitted by low Z elements. These low energy detectors typically have
two windows, an entrance window usually fashioned from a low density organic material, and an exit window

11 You can guess why one author of this book knows this.
Sec. 10.6. Selected Proportional Counter Variations 389

Figure 10.20. (left) Handheld thin-window gas-flow proportional counter (Ludlum 43-68) in
which the thin aluminized boPET window and window guard are visible, and (right) handheld
thin-window gas-flow proportional counter in which the gas and electronic connections are visible.

front thin
window

connector
anode

out back window in

Figure 10.21. Diagram of a thin window pro- Figure 10.22. Photon transmission probabil-
portional counter tube used for detection of low ity for several thin window materials. Data
energy photons. After [Goldstein et al. 1981]. from [Potts 1987].

composed of 25 micron thick Be that helps to reduce the production of secondary radiation (ejected electrons)
from photon interactions with the back wall (see Fig. 10.21).

10.6.2 Sealed Proportional Counters


Sealed proportional counters are available in a variety of geometries, although the most popular configurations
are based on coaxial cylindrical designs. These proportional counters offer an economical method of radiation
detection and come in sizes ranging from 1-cm diameter to several centimeters in diameter and with lengths
of up to 1 to 2 meters. Unlike gas-flow detectors, the detector gas is not replenished, and consequently, the
quenching gas can be depleted over time. Common commercial units are backfilled with H2 , Ne, Ar, Xe, Kr,
P-10, 3 He, or 10 BF3 .
Voltages applied to proportional counters are typically higher than those used for ion chambers; hence,
it is necessary, as with ion chambers, to design the chamber to reduce electronic noise arising from leakage
currents. As discussed in Sec. 9.5.1, a guard ring or guard tube is positioned around the anode wire, as
depicted in Fig. 10.23. The voltage drop across the insulator between the guard tube and anode is effectively
reduced, thereby lowering the leakage current as shown in Fig. 9.25. Leakage currents on the order of 10−16
amps can be achieved with the addition of a guard tube in the chamber [Borkowski 1947].
390 Gas-Filled Detectors: Proportional Counters Chap. 10

outer conductor
outer insulator
field tube middle insulator field tube
rb guard tube
inner insulator
center ra2 i
electrode (ra1) current
voltage meter
Rf
supply
_
+ RL anode insulator
gas-filled chamber virtual ground

Figure 10.23. (left) Diagram of a sealed proportional counter tube with guard ring and field tube, and (right) inside chamber
of a cylindrical steel proportional counter with a field tube.

Figure 10.24. (upper left) Sealed 3 He-filled proportional counter, and (lower left) x-ray image of
the sealed 3 He-filled proportional counter. The Teflon R
insulator standoffs are barely visible in the
x-ray image. (right) Detector response to a collimated thermal neutron beam as a function of position.
The active region of the device is confined to the length between the ends of the standoff connectors,
approximately 42% of the detector length.

The variation in the electric field around the anode near the insulating standoffs can have deleterious
“end-effects” [Cockroft and Curran 1951]. Consequently, the sensitive region within a proportional counter is
not well defined, as shown in Fig. 10.24, In this example, the sensitive region that limits the full development
of the multiplication factor M amounts to only 42% of the detector length. However, the electric field
end effects can be rendered negligible by fitting field tubes over and around the grounded guard tube (see
Fig. 10.23). For a field tube of radius ra2 , the potential is adjusted such that the surface potential is the
same as the radial potential in the gas at radial distance r = ra2 near the detector center. The potential
at the surface of the field tube and the resulting electric field are too small to produce an avalanche. If the
field tube length is approximately the same as the detector radius rb , then the electric field lines emanating
from the anode wire between the ends of the field tubes are also radial with almost no distortion [Cockroft
and Curran 1951].
Other sealed detector geometries include “pancake” detectors, side window detectors, end window de-
tectors, quadrilateral detectors, spherical detectors, straw tube detectors, multi-wire detectors, microstrip
detectors, and position sensitive detectors. A few of these detectors are described below.

10.6.3 Proportional Counters for Low Energy Gamma-Rays


As mentioned earlier, one important use of proportional counters is for detection of low energy x rays,
especially for electron microprobe applications and wavelength dispersive spectroscopy. Such detectors can
Sec. 10.6. Selected Proportional Counter Variations 391

Figure 10.25. Gamma-ray total mass atten- Figure 10.26. Gamma-ray percent absorp-
uation coefficients for common detector gases. tion through a 2.54-cm diameter proportional
Data from [NIST]. counter at 1 atm pressure. Data from [NIST].

be fashioned as gas-flow detectors [Hendee et al. 1956; Dolby 1960; Riggs 1963] or sealed tubes [Lang 1951,
1956; Arndt et al. 1954]. To increase detection efficiency, the detector requires a thin entrance window that
does not appreciably absorb the photons of interest (see Fig. 10.22). Additionally, the fill gas must be able
to absorb the total energy of the photons, an ability that depends on atomic number of the gas, the gas
pressure, and the detector width. Shown in Fig. 10.25 are the photon mass attenuation coefficients μm = ρμ
for noble gases often used in proportional counters. An estimate of the expected intrinsic detection efficiency
I for a collimated photon beam intersecting the detector is
I = 1 − e−μm ρt (10.106)
where ρ is the gas density in g cm−3 and t is the proportional counter tube diameter. Results for several
noble gases loaded into a 2.54-cm diameter tube are shown in Fig. 10.26. Careful selection of the fill gas can
reject high energy photons while giving acceptable detection efficiency of characteristic x rays. For instance,
Ar gas effectively detects characteristic x rays up to approximately 10 keV, while higher energy x rays (>
30 keV) generally pass through the device without detection. As mentioned in a prior section, a thin back
window, usually constructed of Be or perhaps Al, can be used to reduce the probability that these higher
energy x rays interact with the detector walls. Kr or Xe gas can be used to extend the detector sensitivity
to higher energies.
Of special note are the gas K absorption edges that cause a reduction in efficiency at the absorption
energy limit. For instance, the K edges for Ar, Kr, and Xe are 3.208 keV, 14.323 keV, and 34.579 keV,
respectively. Directly below these energies for each respective gas, there is a sharp decrease in efficiency as
can be seen from Figs. 10.25 and 10.26. Additionally, because of the characteristic x-ray transitions among
different shells, energy can be lost from the detector. For instance, electrons excited from the K shell of Xe
have Kα or Kβ transitions of approximately 29.8 keV and 22.64 keV, respectively. If these Xe characteristic
x rays escape the detector, the total energy deposited is reduced by the lost x-ray energy, which results in
the formation of an escape peak in the pulse height spectrum.

10.6.4 Position Sensitive Proportional Counters


A method to turn a cylindrical gas filled detector into a position sensitive detector is described by Kuhlmann
et al. [1966], McDicken [1967], and Borkowski and Kopp [1968]. The basic configuration takes advantage of
392 Gas-Filled Detectors: Proportional Counters Chap. 10

d
V
x d-x
V
I1 R R I2

V1 V2
S
V1 V1 + V2 Total Energy
Deposited
V1 Position of
V1 + V2 Interaction

Figure 10.27. Schematic diagram of a position sensitive gas-


filled proportional counter for the voltage division (charge division)
method.

the distributed resistance of the central anode wire. An avalanche initiated by an ionizing particle causes
current to flow through the anode and can be measured by preamplifiers at each end of the detector (as
depicted in Fig. 10.27). The currents I1 and I2 flowing through the load resistors at each end of the detector
are proportional to the input voltages of each preamplifier. The output voltages from each preamplifier,
V1 and V2 are summed in a circuit to produce a signal that is proportional to the total ionization in the
counter. The quotient of V1 divided by V1 +V2 produces a signal proportional to the location of the avalanche
centroid with respect to the anode.12 Although the configuration and concept are quite simple, the actual
implementation can be somewhat complicated, as pointed out by Fischer [1977]. Regardless, for small
localized avalanches, a spatial resolution FWHM below 1.6 mm is possible [Kuhlmann et al. 1966]. The
position information has been shown to be remarkably linear with the method.
By measuring differences in the risetime of the signals from a detector, spatial resolution below 1 mm
has been reported [Borkowski and Kopp 1968, 1970]. Charge collected from an anode of length d at some
arbitrary position x causes a current to flow through the anode resistance over length x in one direction and
over length d − x in the other direction. The risetime of the input voltage into each preamplifier is a function
of x and is independent of the total charge liberated in the detector. The input voltage is amplified and
shaped with a double RC differentiator to obtain a bipolar pulse, and the risetime of the voltage is measured
by the time of the crossover point of the resulting bipolar pulse. The difference between the risetimes of the
pulses from each end of the detector is a function of the interaction location x [Borkowski and Kopp 1970].

10.6.5 Multiwire Proportional Counters


Multiwire proportional counters (MWPCs), as the name implies, are detectors with several anode wires, and
sometimes several cathode wires, in the same chamber. Developed in 1968 by Charpak, position sensitive
MWPCs use a criss-cross array of wires. Covering large surfaces with layers of classical cylindrical propor-
tional tubes was regarded as impractical,13 and the MWPC concept stems from this perceived limitation.
The original MWPC design consisted of a parallel array of anode wires strung between two cathode planes,

12 The technique has also been used with Geiger-Müller counters by performing the spatial measurement at a preset saturation
threshold VS where VS = V1 + V2 at a set pulse height before the Geiger discharge is fully developed; therefore, the position
x becomes proportional to V1 /VS where VS is approximately constant.
13 This problem was greatly mitigated by the advent of the straw tube detector.
Sec. 10.6. Selected Proportional Counter Variations 393

cathode
plane

cathode plane

anodes
anodes

e- e-
e- e-

cathode plane

cathode
. . amplifiers
....... plane

Figure 10.28. Cross section diagram of a Figure 10.29. Electric field lines in a multi-
MWPC. wire proportional counter (MWPC).

as shown in Fig. 10.28, with the parallel anode wires arranged only a few millimeters apart [Charpak 1970;
Charpak and Sauli, 1979]. During operation, the detector electric field is perpendicular to the cathode
planes, except in the close vicinity of the anodes as seen in Fig. 10.29. In the near field region of the anodes,
the electric field lines must terminate perpendicularly to the anode wire surface, thereby producing a high
electric field similar to a traditional cylindrical proportional counter. As a result, each wire operates as
an individual proportional counter without a grounded barrier between the wires. Georges Charpak was
awarded the 1992 Nobel Prize in Physics for his invention of the multiwire proportional chamber.
Particles entering the detectors produce a track of electron-ion pairs. It is possible with a MWPC to
determine the (x, y, z) coordinates of track of the initial electron-ion pairs. Electrons drift towards the array
of anodes, and when they enter the high field region, they initiate a Townsend avalanche. These electrons
drift into the high field regions of the closest anode wires. The cloud of positive ions from the avalanche
drifts towards the cathode planes, thereby inducing a fast rising current on the anodes from which they are
departing. As discussed in Sec. 10.5.1, the short risetime of the pulse is a fraction to a few microseconds for
most of the induced charge. The pulse is sensed upon those wires closest to the avalanche, thereby localizing
in one dimension, x for instance, the particle track. The y dimension can be determined by connecting each
wire in the same position sensing scheme as shown in Fig. 10.27. Although these anode wires are usually
about 1 to 2 mm apart, the actual spatial resolution achieved is generally less than the wire spacing. Finally
the third z coordinate of the original track location can be deduced from the time required for the electrons
to drift to the anode wire array. A MWPC of this form is commonly referred to as a drift chamber, and is
capable of determining the original track location with sub-millimeter spatial resolution.
Two-dimensional, position-sensitive MWPCs are an advancement on the original design. Typically there
are two planar arrays of parallel cathode wires with the arrays positioned perpendicularly to each other
[Sauli 1994]. One might consider one set of wires parallel to the x direction and the other set parallel to
the y direction. In between the two cathode wire array planes is a parallel planar array of anode wires,
which are typically arranged at a 45◦ -angle to the cathode wires, as shown in Fig. 10.30. As with the simple
proportional counter, ionizing radiation produces primary electron-ion pairs in the detector gas. Electrons
travel towards the nearest anode wires in the array, which then produce a Townsend avalanche of electron-ion
pairs. The cloud of positive ions separates and travels towards the nearest cathode wires in the planes on
394 Gas-Filled Detectors: Proportional Counters Chap. 10

Upper Cathode Delay Line


Wire Array
y output signal
tion
rec
y di
anode
output signal

o
45 Anode Wire
Array
e
Lin
ay
Del de
tho
r Ca ray
e r
Low ire A
W
x output x direction
signal

Figure 10.30. A multiwire gas filled proportional counter is composed of parallel layers
of wire arrays. Shown is a system with three parallel wire arrays, in which the upper
and lower arrays are cathode wires arranged orthogonally. The middle anode array is
arranged at a 45◦ -angle to the cathode arrays.

both sides of the anodes. Hence, the position of the event is determined by which cathode wires deliver a
signal on the x-y plane. Overall, the multiwire proportional counter can provide both energy information
and position information of the ionizing event.
The multiwire concept has been used in a variety of detector designs, including open cell detector designs,
gas-flow alpha particle detectors, and straw tubes. The interlacing of anodes and cathodes in a larger tube
facilitate faster response times from these detectors. For planar devices, such as those shown in Figs. 10.18
and 10.20, the electric field is flattened throughout much of the active region, thereby providing a uniform
response over most the detector area.

10.6.6 Microstrip Gas Chambers


A clever method to produce a microscopic electrode is to pattern the tiny anode upon an insulating substrate.
The process is commonly used for microwave and millimeter wave transmission lines, in which a metallic strip
is placed upon a dielectric substrate. The design has been used to produce compact proportional counters
[Oed 1988].
The microstrip gas chamber (MSGC) is produced by photolithography means, in a similar fashion as
used for semiconductor microelectronics. An insulating substrate, such as glass, precoated with a conductive
metal, such as Cr, Cu or Au, is patterned with a photo sensitive chemical commonly referred to as a
photoresist. A photomask with an image of the desired pattern is brought into close proximity of the
substrate and the photoresist is exposed to ultraviolet light, usually with wavelengths of 360 to 420 nm. The
transferred pattern is then developed on the substrate and the undesired regions of the conductive metal
are etched away, leaving behind micropatterned microstrips. Afterwards, the photoresist is dissolved away,
usually with an organic solvent.
This fabrication method can create microscopic metallic strips on the order of, or smaller than, common
anode wires used in proportional counters and Geiger-Müller counters. The microstrips can be fabricated
with great precision and have widths of about 10 ± 0.2 microns. Wider cathode strips with widths between
90 to 200 microns are also placed on the same substrate adjacent to the anodes, displaced by approximately
5 anode widths [Oed 1988; Workshop 1993]. As shown in Fig. 10.31, these MSPC plates are inserted into a
gas chamber in which the entrance window also serves as the drift cathode.
Sec. 10.6. Selected Proportional Counter Variations 395

window and
drift cathode

electric
gas field lines (a)
region

substrate

anodes cathode strips


back plane (grounded)
window and
drift cathode

electric
gas field lines (b)
region

substrate

anodes insulator cathode plane

Figure 10.31. Cross section diagrams of (a) a gas-filled microstrip propor-


tional counter and (b) a gas-filled micro-gap proportional counter. Typical
dimensions for the anode width are 10 microns. The the MSPC, the cath-
ode strip widths are between 90 and 200 microns with a repetitive pitch
between 200 and 350 microns. The gas-filled region is on the order of 1 cm
thick.

Radiation interactions in the chamber produce electron-ion pairs. The electrons drift towards the anodes,
and when they come into the critical electric field region of the anode, a Townsend avalanche proceeds. The
electrons are rapidly collected and the cloud of positive ions drift more slowly towards the adjacent cathode
strips, thereby creating an induced signal that is input to the amplification electronics. Because of the very
small anode dimensions, the applied potential required to produce an avalanching field is relatively low by
comparison to traditional coaxial proportional counters. Further, the response times of the detectors is
relatively short in the tens of nanoseconds range and are about 2 orders of magnitude faster than traditional
coaxial proportional counters.
These detectors have demonstrated excellent energy resolution for thermal neutron reaction products
when backfilled with a mixture of 3 He and an organic gas, and have a FWHM energy resolution of 1.43%
[Oed 1988]. Further, energy resolution (FWHM) for 13.9-keV characteristic Np x rays from an 241 Am source
was reported to be 18%, and 23% FWHM for 6.4-keV x rays from 57 Co.
Although positive ions drift towards the conductive cathode strips, some positive ions adhere to the
insulating substrate. Those ions that come into contact with the insulating substrate tend to accumulate,
creating a space charge field that, subsequently over time, reduces or negates the avalanching field. To
eliminate space charge buildup, a conductive layer is applied to the back plane of the insulating substrate
and biased at generally the same potential as the anodes. The back plane potential produces a repulsion
field that emerges through the surface of the substrate not coated with conductive metal, thereby effectively
protecting the insulating surface from buildup of space charge from the positive ions.
Another problem encountered in MSPCs is field sparking between the anodes and cathodes. Although
the potential applied to the anodes is relatively low, the electric fields can be quite high and lead to electric
arcing between the closely spaced electrodes. Such arcing can erode or damage the microstrips. One method
to ameliorate the arcing is to apply an insulating polyimide spark guard, approximately 1 micron wide, over
the edges of the cathode strips [Nagae et al. 1992].
396 Gas-Filled Detectors: Proportional Counters Chap. 10

An alternative design to reduce space charge buildup is the micro-gap gas chamber (MGC) [Angelini et
al. 1993]. A pattern of insulating strips are applied on top of a substrate that remains completely coated
with conductive material, as shown in lower part of Fig. 10.31. Because the substrate serves primarily as
a mechanical foundation of the detector, the substrate no longer need be an insulator, and in fact may
be a semiconductor coated with a conductive metal. The micropatterned insulating strips may be applied
by common physical vapor deposition methods, such as evaporation or sputtering, or by chemical vapor
deposition (CVD) methods, such as plasma enhanced CVD (PECVD). The thickness of the insulating strips
is about two microns [Angelini et al. 1993]. Metal patterns serving as the anodes, slightly recessed by a few
microns, are then micropatterned upon the insulating strips. The entire substrate surface of the resulting
device is grounded, thereby preventing the accumulation of positive space charge.
The spectroscopic performance of a MGC is comparable to that of a MSPC, with reported FWHM
energy resolution of 14.8% for 5.4-keV characteristic x rays from Cr. A major advantage of the MGC is
its rapid response time. Because the positive ions travel such a short distance from the anode to cathode,
the response times are on the order of a few nanoseconds comparable to those of semiconductor detectors
[Angelini et al. 1993]. By comparison, common coaxial proportional counters have response times measured
in microseconds, while the MSPC devices have response times approximately 10 times longer than those of
MGC devices.

10.6.7 Straw Tubes


A variation of the sealed proportional counter is the straw tube, so named because the manufactured product
resembles a drinking straw.14 A common method used to fabricate straw tubes utilizes a cylindrical form,
or mandrel, around which thin Mylar R
strips are wound [Baringer et al. 1987; Marzec et al. 2002]. In
some permutations, a 50-micron thick aluminized Mylar R
strip is wound about a 7-mm diameter mandrel.
Afterwards, a 35-micron thick clear Mylar strip is wound and glued over the first strip such that the outer
strip covers the seam of the inner strip. The overlap for rotations is reportedly 2% of the area. After
removal from the mandrel, insulating plugs are inserted into each end of the straw tube, through which a
thin anode wire is threaded. By use of indexing tubules inserted into holes in each plug, the axial location
of the wire is maintained within ±50 microns of center [Baringer et al. 1987].
According to Toki [1990], advantages of a straw tube chamber over multiwire proportional counters
include:
1. They are inexpensive, relatively simple to construct, and robust.
2. The damage caused by anode wire breakage has a minimal effect, because it can be disconnected
without affecting the response of neighboring anodes.
3. Minimal signal cross talk because the straw provides an electrostatic shield between anodes.
4. Electrostatic alignment distortions are minimal (if the anodes are carefully centered).

New methods of manufacture have been introduced, although the straw-tube name continues. For in-
stance, Takuba et al. [2005] describes seamless straw-tube detectors fabricated by painting carbon-filled
polyimide upon a mandrel followed by sintering. Afterwards the seamless tube is removed from the mandrel.
Another reported method uses an ultra-sonic weld and a shaped extrusion method to produce thin copper
tubes [Lacy 2012]. Regardless, the end product is a miniaturized tube with a diameter of 4 to 8 mm that
serves as the cathode shell for a coaxial, gas-filled, proportional counter. Straw tubes can be manufactured
in lengths ranging from a few centimeters to several meters. Straw tubes are often bundled together to form

Precision Paper Tube Company, still in business, is referenced as the manufacturer of aluminized Mylar
14 The R
straw tubes in
many journal articles during the late 1980s and early 1990s.
Sec. 10.6. Selected Proportional Counter Variations 397

a larger tube or compartment to improve overall detection efficiency [Oh et al. 1991; Avery et al. 1993; Basile
et al. 2004].
Thin-wall devices are reported to have been manufactured with two-sided wall thicknesses of less than 25
microns [Toki 1990]. These thin, straw-tube proportional counters are formed into drift chambers to track
particles in high energy physics experiments [Baringer et al. 1987; Ash et al. 1987; Toki 1990]. Vertex tracking
chambers often have hundreds of straw tube detectors arranged in concentric circles. The thin walls of the
straw tubes minimize energy loss as particles pass through the detectors. Further, because so many detectors
are required to build such an instrument, the simplicity of the detectors is economically attractive. Common
gas mixtures reported for use in straw tube detectors include mixtures of Ar, CO2 , C2 H6 , and CH4 [Avery et
al. 1993]. Linear time-to-distance relationships have been observed for gas mixtures of CH4 :CO2 :Ar (4:3:93),
CO2 :Ar (1:4), and ethane:Ar (1:1), each having drift speeds of about 40 to 80 microns/second. Experiments
with C2 H6 /CO2 (1:19) have yielded higher drift speeds but at the expense of non-linear time-to-distance
responses.
Other straw tube designs are under investigation. Recently, multi-anode straw tubes have been introduced
to improve performance of track detectors [Oh et al. 2011]. Straw tubes with B4 C-coated inner walls have
also been explored for neutron detection [Lacy et al. 2011] and are covered in more detail in Chapter 17.

10.6.8 Gas Electron Multiplier


The gas electron multiplier (GEM) was introduced by Sauli in 1997, and is a unique method to produce
high gain in a gas-filled detector [Sauli and Sharma 1999]. In general, a thin insulating film between 50
to 100 microns thick, typically a Kapton R
film, is stretched on a frame and coated on both sides with a
conductive metal (typically Cu). Afterwards, miniature holes approximately 100 microns in diameter are
etched through the metal and insulating film as shown in Fig. 10.32. The GEM is placed in a gas-filled
chamber between cathode and anode plates, usually closer to the anode. When a voltage is applied across
the GEM, a high electric field is formed in each of the holes, high enough to cause ion pair avalanching (see
Fig. 10.33). Typically, the GEM is held at a potential that is positive with respect to the cathode plate and
negative to the anode plate.
When an ionizing particle enters the gas detector between the cathode and GEM, primary electron-ion
pairs are created as in a typical ion chamber or proportional counter. The electrons drift towards the GEM
and the positive ions drift towards the cathode. When electrons reach the GEM, they are funneled into the
tiny holes where avalanching gas multiplication occurs. Hence, a much larger cloud of electrons emerges from
the GEM with gains up to 200. These electrons continue to drift towards the anode where they induce an
output signal. By using several GEMs in stages, much higher gains can be achieved, often exceeding 1000.
Position sensitive GEMs can be manufactured by using segmented anodes. Various additional coatings on
top of the actual GEM conductor coatings can make the GEM more sensitive to gamma rays and neutrons.
For instance, a GEM coated with Gd, 10 B, or 6 LiF is sensitive to neutrons, while a GEM coated with CsI
or NaI will have enhanced sensitivity to gamma rays.

10.6.9 Neutron-Sensitive Proportional Counters


Gas-filled proportional counters designed for neutron detection are briefly described in the present section.
A detailed discussion of gas-filled neutron detectors is reserved for Chapter 17.
Detectors based on Neutron Reactive Gases
The most commonly used materials in proportional counters that can detect neutrons are the gases 3 He and
10
BF3 , and the solid 10 B. Although neutron sensitive, neither 10 BF3 nor 3 He are ideal proportional gases, but
they perform adequately well. Because the device operates in proportional mode, a low resolution spectrum
associated with the reaction product energies of the 10 B(n,α)7 Li reactions or the 3 He(n,p)3 H reactions can
398 Gas-Filled Detectors: Proportional Counters Chap. 10

Figure 10.32. A scanning electron microscope


photograph of a GEM section, showing the Kap-
ton film, the Cu conductive surfaces, and the
holes. The holes in the present photograph are Figure 10.33. The electric fields around and
approximately 75 microns in diameter. From in holes of a GEM detector. From Sauli [2016].
Sauli and Sharma [1999]. Courtesy F. Sauli. Courtesy F. Sauli.

be identified, depending on the gas used in the counter. The neutron detection efficiency can be increased
by increasing the gas pressure of the counter so that there is more neutron absorber. Typical pressures
for 3 He detectors range from 1 atm to 10 atm. Electron and ion speeds decrease inversely proportional to
gas pressure and, consequently, increasing the gas pressure in the tube causes the dead time of the counter
to increase. Gas-filled tubes come in a variety of sizes, ranging from only a few centimeterslong and one
centimeter in diameter to several feet long and several inches in diameter.

Detectors based on Neutron Reactive Inserts


A traditional proportional gas may be used in the chamber, such as P-10, if instead of filling the chamber with
a neutron reactive gas the walls are coated with 10 B. Unfortunately, the spectral features from such a device
are harder to interpret due to interference from background gamma rays, and the total neutron detection
efficiency is limited by the optimum 10 B absorber thickness, typically only 2 to 3 microns. The detectors
are made more efficient by increasing the tube diameter, or by inserting additional 10 B-coated plates in the
chamber. Neutron reactive inserts can also be introduced into the proportional counter, for example 6 Li
blades. These detectors can be designed to preserve the reaction product spectra while delivering efficiencies
competitive with detectors backfilled with 3 He or BF3 [Nelson et al. 2012].

10.6.10 Selected Planar Proportional Counters


Finally there are several very specialized proportional counters that include detectors such as micro-mesh
gaseous detectors (MicroMegas detectors) and resistive plate chambers (RPCs). The MicroMegas detector
consists of a basic planar gas-filled chamber, on the order of 3 mm wide, that resembles the construction of
a Frisch grid ion chamber [Giomataris et al. 1996]. The grid, or mesh, is located near the anode, usually
within 100 microns. The voltage applied between the cathode and mesh drifts electrons towards and through
the mesh (∼ 103 V cm−1 ). The voltage applied to the region between the mesh and the anode produces
an electric field above the critical field Et required for avalanching (> 105 V cm−1 ), and therefore, produces
a Townsend avalanche. The resulting positive ions liberated in the avalanche are subsequently collected by
the mesh electrode. Clever anode designs allow for MicroMegas detectors to be used as a position sensitive
proportional counters [Derré and Giomataris 2001]. MicroMegas detectors are used as high-energy particle
tracking detectors [Titov 2007].
Problems 399

The RPC is another planar style proportional counter dependent upon narrow gas-filled gaps. The basic
construction has two parallel resistive plates, between which is a narrow gas-filled gap, which is usually a
few hundred microns wide [Santonico and Cardarelli 1981; Cardarelli et al. 1988]. The resistivity of the
materials is reportedly to be about 1010 to 1012 Ω-cm [Cardarelli et al. 1988]. A conductive electrode is
applied to the outer surfaces of the insulators. A voltage applied across the detector will drop some voltage
across the resistive materials; however, due to the high resistance of the gas-filled gap, most of the applied
voltage appears across the gap, thereby producing an electric field above the critical electric field required
for avalanching. Although there is signal reduction due to the capacitance of the resistive plates [Bacci et al.
1995], the increased signal from the avalanche is ample for detection. RPCs have reported timing resolution
of around 100 ps [Santonico 2003]. Because the narrow gap absorbs little energy from the radiation particles
of interest, these detectors generally consist of numerous RPCs in a stack. Patterned electrode designs and
stacked configurations allow for the realization of relatively small position sensitive counters [Couceiri et al.
2007], with reported spatial resolution of 500 microns after the application of a reconstruction algorithm.

PROBLEMS
1. The electronic output from a cylindrical gas-filled chamber is primarily dominated by electron current
when operated as an ion chamber. When operated as a proportional counter, the electronic output from
the same detector becomes dominated by positive ion current. Explain why this change occurs.

2. A coaxial detector is backfilled with P-10 gas to 2 atm. The detector has anode wire with a radius of
25 microns and cathode radius of 1.5 cm. Determine rc for an applied voltage of 1500 volts.

3. Use Stirling’s approximation to prove that Eq. (10.102) becomes the Poisson distribution as θ → ∞.

4. Verify that the solution of Eq. (10.84) is given by Eq. (10.85).

5. Show that the second moment of Eq. (10.91) is m2  = 2m2 − m.


%
6. Verify (a) that the Furry PDF of Eq. (10.88) is properly normalized, i.e., ∞
m=1 p(m|a) = 1, (b) the first
moment m = exp[τ (a)], (c) the second moment is m  = 2m − m, and (d) the relative variance
2 2

is given by Eq. (10.92).

7. You have a coaxial detector with ra = 25 microns and rb = 12.5mm. The tube is pressurized to 1.5
atm with a mixture of 90% Xe/ 10% CH4 . What voltage must be applied to the anode to just barely
produce a gas multiplication of M = 20?

8. A coaxial detector has ra = 25 microns and rb = 15 mm, and is backfilled with P-10 gas at 2 atm.
The operating voltage is 1000 volts. A 5.5 MeV alpha particle interacts in the detector, producing an
ionization trail parallel to the anode at a random distance r from the center. Approximate the time
after the event (tVmax /2 ) that 50% of the induced pulse is produced. How far did the ions travel to
produce this pulse? You now change the gas pressure to 0.5 atm. What are the new values of (tVmax /2 )
and the travel distance?
400 Gas-Filled Detectors: Proportional Counters Chap. 10

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SAULI, F., Gaseous Radiation Detectors, Cambridge: Cambridge Progr. Nucl. Phys., O.R. FRISCH, Ed., 3, 18–62, (1954).
University Press, 2014.
WIJSMAN, R.A., “Breakdown Probability of a Low Pressure Gas
SAULI, F., “The Gas Electron Multiplier (GEM): Operating Prin- Discharge,” Phys. Rev., 75, 833–838, (1949).
ciples and Applications,” Nucl. Instrum. Meth., A805, 2–24,
WILKINSON, D.H., Ionization Chambers and Counters, Cam-
(2016).
bridge: University Press, 1950.
SCHLUMBOHM, H., “Zur Statistik der Elektronenlawinen im Ebe-
WILLIAMS, A. AND R.I. SARA, “Parameters Affecting the Reso-
nen Feld. III,” Z. Physik, 151, 563 (1958a).
lution of a Proportional Counter,” Int. J. Appl. Radiation
SCHLUMBOHM, H., “Zur Statistik der Elektronenlawinen im Pro- Isotopes, 13, 229–238, (1962).
portionalzählrohr. IV,” Z. Physik, 152, 49 (1958b).
WOLFF, R.S., “Measurement of the Gas Constants for Various
SIMPSON, JR., J.A., “Proportional Counter,” US Patent 2532956 Proportional-Counter Gas Mixtures,” Nucl. Instrum. Meth.,
A, allowed May 2, 1950a. 115, 461–463, (1974).
SIMPSON, JR., J.A., “Air Proportional Counter,” US Patent Workshop on Progress in Gaseous Microstrip Proportional
2532956 A, allowed Dec. 5, 1950b. Counters, Conf. Rec., Grenoble, 1993.
SIPILÄ, H., “Energy Resolution of the Proportional Counter,” ZASTAWNY, A., “Gas Amplification in a Proportional Counter with
Nucl. Instrum. Meth., 133, 251–252, (1976). Carbon Dioxide,” J. Sci. Instrum, 43, 179-181, (1966).
SNYDER, H.S., “Fluctuations for Proportional Counters.,” Phys. ZASTAWNY, A., AND J. MIZERACZYK, “Gas Gain in a Proportional
Rev., 72, 181, (1947). Counter Filled with Argon and Nitrogen,” Nukleonika, 11, 685–
689, (1966).
SPIELBERG, N., “Effect of Anode Material on Intensity Dependent
Shifts in Proportional Counter Pulse Height Distributions,” Rev. ZASTAWNY, A., “On a New Formula for the Gas Amplification in
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Chapter 11

Gas-Filled Detectors:
Geiger-Müller Counters
The sudden current through the gas due to the entrance of an
α-particle in the testing vessel was thus increased...
Sir Ernest Rutherford and Hans Geiger

Although Hans Geiger originally created the gas-filled detector in 1908 (with Ernest Rutherford) [Rutherford
and Geiger, 1908],1 the “Geiger” counter in wide use today is based on an improved version that his first
PhD student, Walther Müller, constructed in 1928 [Geiger and Müller 1928a, 1928b, 1929a, 1929b]. Hence,
the proper name for the device is the Geiger-Müller counter. The original “Geiger” counter was sensitive
to alpha particles, but not so much to other forms of ionizing radiation. Müller’s improvements included
the utilization of vacuum tube technology to create a device that was compact and portable and that was
sensitive to alpha, beta, and gamma radiations. In 1947, Sidney Liebson further improved the device by
including in the tube gas a small amount of a halogen as a quenching gas, an improvement that allowed the
detector to operate at lower applied voltages and to last significantly longer [Liebson 1947a, 1947b].

11.1 Geiger Discharge


Geiger-Müller counters are operated in region IV of the pulse height curve for gas detectors as shown in
Fig. 11.1 and depend upon gas multiplication for signal amplification, much like proportional counters do.
However, a single important difference is that, at any specific applied voltage, all output pulses from a Geiger-
Müller counter have the same amplitude regardless of the energy or type of incident ionizing radiation. Hence,
Geiger-Müller counters cannot discern any difference among alpha, beta, or gamma radiations, nor can they
distinguish among different energies of these radiations. To understand the reason for this behavior, it is
important to understand the progression of the Geiger discharge.2
Geiger counters typically have a coaxial configuration, in which a thin anode wire is placed on the
axis of a cylindrical tube that serves as the cathode. A high voltage is applied to the central anode wire,
while the cathode is held at ground potential, as depicted in Fig. 11.3. When an ionizing particle enters
a Geiger-Müller counter, the counting gas becomes locally ionized in which a small cloud of electron-ion
pairs is formed as depicted in Fig. 11.2(1) and described in the previous chapter. Because a high volt-
age is applied to the anode and the tube is operated in region IV of the gas curve, the electrons drift
rapidly to the anode while the ions slowly drift towards the cathode, as shown in Fig. 11.2(2). When the
electrons enter the high electric field near the anode above the critical field strength Et needed to produce

1 Hans Geiger was nominated for the Nobel Prize in physics three times, in 1935 by Walther Nernst, in 1937 by Walther Bothe,
and in 1955 by Boris Rajewsky, but never received it.
2 A Geiger discharge consists of multiple Townsend avalanches.

403
404 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

ion pair recombination


occurs before collection
avalanche ionization, they gain enough kinetic energy
Geiger-Muller
to produce more electron-ion pairs through impact ion-
onset of region
“gas multiplication”
ization, and a large and dense cloud of electron-ion
transition pairs is formed around the anode. Some of these en-
Pulse Height or Ions Collected

region
LLD ergetic electrons lose energy, through bremsstrahlung,
recombination, or de-excitation, processes that lead to
(log scale)

I II III the production of UV photons which, in turn, cause


more ionization in either the cylinder gas or from in-
teractions with the cathode wall. These newly freed
a particles
electrons form new avalanches and yet more positive
space charge builds up around the anode. This large
IIIa IV V accumulation of positive ions around the anode reduces
the electric field near the anode as depicted in Figs.
b particles 11.2(3) and (4). There comes a point when the large
accumulation of space charge around the anode is so
Detector High Voltage (volts)
high that the electric field is reduced below the criti-
Figure 11.1. Geiger-Müller counters are operated in re- cal field strength Et needed to sustain avalanching. At
gion IV of the pulse height curve for gas-filled detectors. this point the impact ionization ceases, as shown in
The LLD is set to discriminate pulses produced in the pro-
portional and lower regions.
Fig. 11.2(5). The positive ions then slowly drift to-
wards the cathode where they are collected and pro-
duce the signal pulse for the detector. As they reach the cathode, the electric field near the anode recovers to
full strength, and the detector is set to detect the next radiation interaction event, as depicted by Fig. 11.2(6).
Several features about the progression of the Geiger discharge should be noted. (a) The electric field in
the detector increases with increasing applied voltage. (b) The discharge ceases when the electric field is
reduced below Et at the anode and, therefore, the required space charge to terminate the avalanching must
also increase with applied operating voltage. (c) To prevent more electrons from being ejected when the ions
strike the cathode, thereby preventing another avalanche, a form of quenching must be used. (d) The entire
Geiger discharge process is slower than that of a proportional counter, mainly due to the longer time required
to produce the dense cloud of positive ions around the anode. (e) Finally, the size of the output pulse is
determined by how much space charge must accumulate to reduce the electric field below Et and not by the
initial energy absorbed or number of initial electron-ion pairs produced within the detector! Consequently,
the pulse height for various energies of α-particles, β-particles, and γ-rays are all the same, within statistical
variation, and the signal pulse height is predetermined solely by the applied operating voltage.

11.2 Basic Design


The basic design of a Geiger-Müller (G-M) counter is shown in Fig. 11.3 and consists of a coaxial chamber
that serves as the detector cathode and the anode is threaded into the chamber through an insulator. The
anode is small in diameter, yet robust enough to be rigidly suspended in the tube. Typically, wire diameters
on the order of 100–200 microns can achieve the desired electric field. Thinner wires can be used if suspended
by both ends. An insulating glass bead is attached to the anode wire, which helps stabilize the electric field
at the end of the anode.
Older versions of G-M counters were constructed from glass envelopes, and a metal sleeve was inserted
into the chamber to act as the cathode. The choice of cathode material affects the gamma-ray response of
the chamber. High Z materials, such as Pb or Bi, have a fairly salient “over response” to gamma-ray energies
below 500 keV (as discussed later in Section 11.5.3). Present day G-M counters are usually constructed from
a stainless steel cathode tube without any such inserts, and rely on the stainless steel tube for gamma-ray
interactions.
Sec. 11.2. Basic Design 405

initially, no space charge


cathode
|E| |E|
slow
ions + Et + moving ions Et
+ +
+ electrons +
Townsend
anode r Avalanche
r

1. Primary event creates ion pairs. 2. Electrons rapidly drift to the anode and
cause a Townsend avalanche - which creates
a tremendous number of ion pairs.
|E| |E|
+ + +
+ + Et Et
++ ++ + +
+ +
+
+ +
+
++ + + + ++ +
+ + + r + + + +
+
r
+ ++ + +
+ + +
+ + +

3. UV light from excited atoms in the avalanche 4. Waves of avalanches occur from the ion pairs
excite more ion pairs. excited by released UV light. Positive space
charge begins to build up around the anode.
E raises back
|E| E reduces below Et |E| above Et
- avalanching stops + +
+
+ +
+ + +
++ + Et +
+ + + + + + Et
+ +
+ +
+ + + +
+ + +
++ + +
+ + ++ +
+ +
+ ++ + + +
r + + + + +
+
r
+
+ + + ++ + + +
+ + + + + +
+ + + +
+ + +
+ + + +

5. Positive space charge builds up around the 6. The space charge drifts away from the
anode to the point that the electric field is anode towards the cathode (wall). The electric
reduced below the critical value for avalanching. field recovers such that another Geiger
The avalanching ceases. discharge can occur.

Figure 11.2. Geiger-Müller tube cross section depicting the progression of the Geiger
discharge. The avalanching continues until the space charge accumulated around the
anode wire decreases the electric field below the avalanche threshold, which then causes
the progression to cease.

Chamber
Glass Bead Anode Insulator

Anode out Screen


Seal

Rch
RL
Fill Gas

- +
Window Chamber (Cathode)

Figure 11.3. (left) simplified circuit for a G-M counter, and (right) the basic components of a
G-M tube.

Because α and β particles cannot penetrate thick-walled G-M tubes, a thin entrance window is usually
used to seal the end of the tube, thereby making a cantilevered anode wire essential. The window is usually
made of either aluminized boPET or mica. The gas inside the G-M tube is under a mild vacuum (commonly
between 0.1–0.2 atm) in order to reduce the detector dead time [recall Eq. (9.31)]. To prevent damage or
contamination, many manufacturers of G-M tubes provide a protective screen over the entrance window.
406 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

Figure 11.4. First ionization energies of the elements. Common gases and cathode
materials that have been used in G-M counters are identified by their chemical symbol.

Care should be taken with G-M tubes and the ambient external pressure. At some altitudes, the external
pressure can be lower than the internal tube pressure, thereby pressurizing the tube and causing a rupture
in the window. Manufacturers usually document such restrictions on specification sheets.

11.3 Fill Gases


Although a variety of gases have been successfully used in G-M counters [Korff 1946; Sinclair 1956; Price
1963; Emery 1966], most often the host gas is one of the noble gases. From Fig. 10.10, neon allows the
highest electron drift speeds, followed by those of He and Ar. Neon also has one of the highest ion drift
speeds of the noble gases, second only to that of He [Munson and Tyndall 1941, Sharpe 1964, Barsuto et
al. 2000].3 Hence, Ne is usually the gas of choice, mainly because it helps reduce dead time by allowing the
dense ion cloud to form more rapidly and to sweep out more rapidly the positive ions. However, Ne also has
a higher first ionization coefficient (and higher average ionization energy) than Ar, although lower than that
of He, as can be seen from Fig. 11.4. Thus, a higher specific ionization per unit length of electron travel is
achieved in Ne than in He, while retaining a faster response than that of Ar. However, often a small amount
of Ar is added to the gas to increase the specific ionization while still retaining a fast signal response.
There may be special applications where high atomic number noble gases are used in G-M counters,
although this practice is uncommon. Under such conditions, it is possible for low energy gamma rays to
interact directly with the gas. As can be seen from Fig. 10.26, high efficiencies can be achieved for gamma-ray
energies below 30 keV. However, the electron velocities for Kr and Xe are significantly lower than those of
Ne and Ar (see Fig. 10.10), as well as the ion mobilities [Munson and Tyndall 1941], thereby causing these
G-M counters to have longer dead times.
Because of the large ionization clouds produced in G-M tubes, it is necessary to include a quenching gas
along with the host detection gas inside sealed tubes. Organic polyatomic gases work well in G-M tubes, but
these gases can be consumed after several months of continuous use as the molecules dissociate irreparably.
Instead, it is a usual practice to use diatomic halogen gases to quench the Geiger discharge because these
gases undergo a form of self-repair after dissociation.

3 Recall from Fig. 10.10 that Ne has the highest electron drift speed of the noble gases.
Sec. 11.3. Fill Gases 407

11.3.1 Quenching
If a G-M tube is operated with a pure counting gas such as argon or neon, positive ions drifting to the
cathode attract electrons to the surface, and upon contact, an electron from the wall neutralizes the positive
ion. Ideally, the atom is neutralized and the collection process simply ends. However, the actual process is
considerably more complicated.
When a gas ion comes into contact with the cathode wall, the absorption of an electron leaves the now
neutralized atom in an excited state. This physical state occurs because of the differences in ionization
energies between the gas atoms and the cathode atoms. Typically, a noble gas atom de-excites by releasing
a photon with an energy comparable to the atom ionization energy. For example, the minimum ionization
energy for Ar is 15.6 eV, corresponding to a photon wavelength of 78.47 nm and classified as belonging to
the extreme ultraviolet (EUV) region of the electromagnetic spectrum. Almost all transition metals have
minimum ionization energies ranging between 5–10 eV, as can be seen from Fig. 11.4. Consequently, if
the EUV photon strikes the wall, a photoelectron may be ejected, thereby triggering another Townsend
avalanche. Due to competing processes, the actual photo-efficiency for these UV photons is actually very
small, on the order of 10−4 per photon [Korff 1946]. However, the number of electron-ion pairs produced
for a single event and in the subsequent discharge usually produces many more than 104 electron-ion pairs
per event so that there is an appreciable probability that a photoelectron is emitted from the cathode wall
because of the absorption in the wall of a UV photon.
With sufficient excitation, it is also possible for atoms of the host gas to release, or excite, K-shell
electrons. Further, it is possible that the host gas becomes multiply-ionized. By recombination and de-
excitation, energetic x-ray photons can be emitted. For example, Ar photon emission energies can be over 3
keV (Kβ = 3.192 keV; Kα1 = 2.957 keV). Also, excited neutral gas atoms can emit one or more characteristic
x rays. These characteristic photons have sufficient energy to cause direct ionization of the atoms of the host
gas and, consequently, increase and prolong the avalanching process.
It is also possible for a gas ion, with sufficient kinetic energy, to directly cause the emission of an electron
when it comes into contact with the cathode wall. The ejected electron then sets off another Geiger discharge.
In all these cases, there is a release of an electron that can cause another Geiger discharge, which is easily
mistaken for another radiation interaction event, unless a mechanism is employed to prevent (quench) the
release of another electron, or at least to render such secondary electrons incapable of starting another Geiger
discharge. Geiger-Müller detectors are considered to be either “non-self-quenching” or “self-quenching” [Korff
1946]. Quenching in a non-self-quenched detector relies upon a combination of space charge accumulation
and external resistance to terminate and quench the Geiger discharge. By contrast, self-quenching G-M
detectors have a quenching gas added to the detection gas to prevent electron ejection by positive ions.

Non-Self-Quenching Detectors
Consider the circuit shown in Fig. 11.3, in which the potential across the detector is produced by a resistive
divider, formed by the load resistor RL and the chamber resistance Rch . Because the chamber is filled with
a neutral gas, Rch RL . After a radiation particle enters the chamber and initiates a Geiger discharge,
current from electron collection begins to flow through the anode wire, and also through the load resistor,
thereby causing the voltage drop across RL to increase at the expense of the voltage held across the chamber
[Werner 1934a, 1934b]. As the Geiger discharge increases, so does the electron current and the space charge
sheath surrounding the anode, until eventually the voltage held in the chamber falls below the threshold
potential required to sustain a Geiger discharge. When the falling potential reaches a value such that the
electric field at the anode surface falls below Et , the Geiger discharge terminates. Although this termination
method was initially called “quenching resistance,” Montgomery and Montgomery [1940] argue that a high
load resistance actually prolongs the Geiger discharge, because the current leakage through RL allows the
408 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

anode wire to maintain its original potential for a longer period of time;4 hence, it is mainly the space charge
accumulation that stops the Geiger discharge and not the voltage reduction produced by the load resistance.
Typically, it is multiple cascades of electrons liberated from the cathode wall by UV photons that builds
up the Geiger discharge. Montgomery and Montgomery [1940] report the observed formation of multiple
discharges until the space charge sheath eventually terminates the progression. Regardless, if RL > 108 Ω,
then the RC time constant of the chamber and circuit is usually longer than the collection time of the
ions, thereby allowing collection of the positive ions before the chamber resets. In other words, the detector
recovery time is longer than the positive ion collection time. Hence, any electrons ejected from the cathode
during the recovery time cannot cause another Geiger discharge. This method of quenching is seldom, if
ever, used in modern Geiger-Müller counters, mainly because these detectors suffer from long resolving times
(≥ 10 ms), thereby limiting their use to low radiation fields.

Self-Quenching Detectors
The almost universal method used today for quenching G-M counters is to add a small amount of quenching
gas to the main detection gas. Polyatomic organic gases were initially used with much success, as described
earlier in Chapter 10 for proportional counters. One function of polyatomic organic gases in the mixture is
to absorb the UV photons emitted by excited atoms of the primary gas. Without the quenching gas, these
photons would produce additional ionization in the detector gas or cause photoemission of electrons from the
cathode wall. Upon absorption of a UV photon, a polyatomic molecule, with relatively weak molecular bonds,
generally dissociates before the absorbed energy can be emitted in the form of photoelectrons or photons.
This dissociation causes a dramatic reduction in the number of UV photons that reach the cathode. Further,
if the polyatomic gas has a lower ionization potential than the primary detector gas, electron exchange can
take place such that the detection host gas ion is neutralized and the polyatomic molecule becomes ionized.
When an ionized polyatomic gas molecule strikes the cathode, it becomes neutralized, and the excited state
of the molecule causes dissociation rather than photon emission, thereby preventing electron emission from
the cathode wall. The three major quenching processes are depicted in Fig. 11.5.
Neon is perhaps the most popular counting gas used in Geiger-Müller counters, followed by argon. Suc-
cessful organic quenching gases include CH4 (methane), C2 H5 OH (ethyl alcohol), and C3 H6 O2 (ethyl for-
mate), often added as 10% of the total gas concentration [Sinclair 1956]. Because G-M counters are typically
closed tubes, the organic quenching gas inside can be exhausted over time, eventually leading to sporadic
counts as the quenching gas is exhausted. Higher voltages require more space charge to stop the Geiger dis-
charge and, consequently, reduce the lifespan of tubes using organic quench gases. Also, using these counters
in relatively high radiation environments reduces the lifetime of the quench gas. It has been reported that
the expected life of an organically quenched counter is  1010 counts [Spatz 1943], in which approximately
109 molecules are destroyed per discharge [Price 1963].
The discovery that halogens also act as quenching gases for Geiger-Müller detectors led to their popular
use [Liebson 1947a; Liebson 1947b; Present 1947; Liebson and Friedmann 1948]. Halogens, unlike organic
gases, appear to undergo a healing recombination reaction back into diatomic molecules, thereby extending
the lifetime of the quenching gas in the detector. Only low concentrations of halogens are needed to effect
the quenching process, usually less than 1% of the total gas concentration [Sinclair 1956]. Reported gas
mixtures include Ne or Ar as the primary counting gas with 0.1% of either Cl2 or Br2 gas added.
There are performance differences between organic and halogen quenched Geiger-Müller counters. For
example, the required operating voltage of a halogen quenched detector is significantly lower than that of an
organic quenched detector. Typical operating voltages for halogen quenched G-M tubes range from 250–700
volts, whereas the same tube quenched with an organic gas may require well over 1000 volts for operation.

4 Korff [1946] suggested that a better name would be “recovery resistance”.


Sec. 11.3. Fill Gases 409

cathode
wall
ionized
gas atom

+ UV photon
excited emission
neutral atom
- photoelectron

(a)
cathode
wall

+
ionized gas excited
molecule neutral dissociation
molecule

1 2 3

cathode
wall
ionized
gas atom neutral
atom
+
- electron

(b)
cathode
wall
neutral
molecule
+
ionized gas
molecule dissociation

1 2

neutral photo
atom + ionization

photon - photoelectron

(c) neutral
molecule excited
neutral
molecule
dissociation
photon

1 2 3
Figure 11.5. Quenching mechanisms of polyatomic gas molecules. In (a), an ionized
gas atom comes into contact with the wall and neutralizes into an excited state. De-
excitation produces an energetic photon that can eject photoelectrons from the cathode.
However, excited gas molecules (organic or halogen), de-excite through dissociation and
do not release additional electrons. Other processes of gas quenching through molecular
dissociation are depicted in (b) and (c).
410 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

Also the plateau length of a halogen quenched G-M tube is usually shorter than one quenched with an
organic gas, often having a plateau range no more than 150 volts. Further, the plateau slope is usually
larger, typically on the order of a 10% increase over the plateau range.
Halogens are reactive oxidizers for many materials and this property can lead to corrosion over time of
internal detector components. Although the concentration of halogen gas is small, caution is still necessary
in selecting materials for the cathode and anode. Stainless steel as the anode and cathode has proven to
work well with halogen quenched G-M counters and is frequently used in modern G-M counters. A popular
choice of stainless steel for halogen quenched G-M counters is 446 SS (about 27% Cr, 73% Fe), a stainless
steel with perhaps the best corrosion resistance of the Cr alloys.

Example 11.1: Consider a Geiger Müller tube pressurized to 0.2 atm filled with Ne and 10% CH4 . The
tube has a diameter of 4 cm and a length of 15 cm. Estimate the number of counts that can be recorded
before the quench gas is exhausted. Assume recombination of dissociated molecules is negligible.

Solution:
From the ideal gas law, the number of mols of gas in the tube is n = P V /(RT ) where the gas constant
R = 0.0821 L atm K−1 mol−1 is
PV (0.2 atm)(π(2 cm)2 (15 cm))
n= = = 1.53 × 10−3 mol.
RT (0.0821 L atm K−1 mol−1 )(300 K)
The number of quench gas molecules NCH4 initially in the tube is

NCH4 = 0.1(nNa ) = 0.1(1.53 × 10−3 mol)(6.022 × 1023 molecules mol−1 )


= 9.21 × 1019 CH4 gas molecules.

where Na is Avogadro’s number.


If 109 quench molecules dissociate for each count, then the counter can have a maximum of 9.21 × 1010
counts before the quench gas is completely exhausted. In reality, the side effects of losing the quench
gas molecules appear much earlier, manifested as an increase in counting plateau slope and the increasing
appearance of sporadic counts.

11.4 Pulse Shape


Because the Geiger discharge produces a large signal voltage, Geiger-Müller counters can be operated without
amplification circuitry, a clear advantage over other types of gas-filled detectors. The shape of the signal
voltage pulse produced by a G-M counter is defined by the rise time and decay time of the detector.5 The
rise time constant is determined mainly by the load resistor and detector capacitance (see Fig. 11.3). There
is a time delay between the initial ionizing event and the start of an avalanche, a delay that depends mainly
on the electron drift speed and tube radius. The lighter high-mobility noble gases, such as He and Ne, have
much shorter time delays than those in the heavier noble gases such as Kr and Xe. Hence, the observed
signal pulse begins slightly after the radiation interaction, a delay of a few microseconds for low electron
mobility gases.6

5 The input voltage Vin is defined as the signal transferred from the detector to the initial amplification stage of a preamplifier,
whereas the output voltage Vout is the output signal of the preamplifier. Because G-M counters are often operated without a
preamplifier, the term “signal voltage” is adopted here for pulses produced by a G-M detector.
6 For most applications, this fact is of little consequence. However, if one wishes to use a G-M counter for timing purposes, the

delay time between the ionizing event and the pulse trigger must be taken into account.
Sec. 11.4. Pulse Shape 411

The actual pulse from a G-M counter, during the progression of the Geiger discharge, develops from
multiple avalanches. These avalanches eventually cause the space charge sheath to completely cover the
anode wire. The electrons are rapidly collected, but contribute little to the signal pulse. It is instead the
motion of positive ions towards the cathode that produces almost all of the signal. Recall from Chapter 10
that most of the induced signal from a coaxial detector is formed within the first few microseconds of ion
drift. Hence, a load resistor is chosen to yield a time constant of a few microseconds.
A coupling capacitor between the load resistance and
recording electronics effectively blocks DC current from
the detector, while allowing signals to pass through. The
signal continues to increase as the positive ions drift to
the cathode; however, the slow motion of ions causes a
slow rise in signal. The coupling capacitance is chosen
to ensure that the decay time constant is sufficiently
large to reduce signal attenuation, while still allowing
reasonable count rates.
Consider the pulse shapes of Fig. 11.6. Large cou-
pling capacitances increase the total pulse height, but
also produce long decay times and, consequently, pro-
duce large dead times. Low coupling capacitances
shorten the decay time and dead time, at the expense Figure 11.6. Depiction of Geiger-Müller tube signal
of a reduced pulse height. Although the signal is low- pulse shapes for different differentiating RC time con-
ered by reducing dead time, it is of minor consequence, stants.
mainly because the ion density developed in a G-M counter is large to begin with so that a reduction in pulse
height can be tolerated. Finally, because the space charge sheath needed to terminate the Geiger discharge
is nearly the same (at a given operating voltage), then the signal pulses are also nearly the same, within
statistical fluctuations.

11.4.1 Dead, Resolving, and Recovery Times


Immediately following the Geiger discharge, the space charge sheath formed around the anode wire lowers
the electric field such that avalanching ceases. Not until the electric field at the anode recovers above the
critical avalanching threshold field Et can another Geiger discharge occur. As the positive ions drift away
from the anode, the electric field at the anode begins to increase, as depicted in Fig. 11.2. The dead time is
the time interval between the initial pulse trigger and the electric field recovery to Et and depends strongly
upon the number of ions in the space charge sheath. In other words, the dead time is dependent upon the
applied operating voltage. Dead times for Geiger-Müller counters can be on the order of 10 times longer than
those of proportional counters of similar size, typically 80–300 microseconds, and represents the minimum
time required between the arrival of successive incident radiation particles that allows their detection. The
longer dead times associated with Geiger-Müller counters are a consequence of relatively long pulse formation
process depicted in Fig. 11.2.
Although it is theoretically possible to register a count after the electric field has recovered to Et , Geiger-
Müller counters are almost always operated with the LLD set to exclude electronic noise; hence, counts
cannot be registered until the resulting pulse height surmounts the preset LLD threshold. The resolving
time is the interval between the initial pulse trigger and when the pulse height reaches the LLD threshold.
Clearly, the resolving time is a function of both the applied voltage and the preset LLD threshold; therefore,
the resolving time is not an intrinsic feature of the detector, but instead changes with the operator’s LLD
setting. It is the resolving time that is usually reported as the detector dead time, although in the strictest
412 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

  sense it is not the dead time, although it certainly has the same
  effect. Overall, count rates from a G-M counter are affected
  principally by the resolving time of the instrument.
The recovery time is defined as the interval between the initial
pulse trigger and the time that another pulse signal can achieve
the maximum amplitude possible. Intuitively, one might sur-
mise that the recovery time is synonymous with the positive ion


collection time; however, as explained previously for non-self-


quenching detectors, the signal tail is also a function of the RC
 


time constant of the detector. Hence, for a large load resistance
RL , the recovery time is a function of both the ion drift time and
the detector time constant. Signal pulses formed during the time
interval between the resolving time and the recovery time have

lower amplitudes than those produced by a full Geiger discharge.
Figure 11.7. Illustration of dead, resolving, Shown in Fig. 11.7 is an illustration of the relation between dead,
and recovery times with respect to signal pulses resolving, and recovery times from a G-M counter.
for a Geiger-Müller tube.

11.5 Radiation Measurements


Although there are multiple variations and uses of Geiger-Müller counters, it is customary to determine first
a proper operational voltage for the devices. This calibration process usually requires radioactive sources to
determine the appropriate LLD setting and the boundaries of the counting plateau. G-M counters cannot
distinguish among different types of incident radiation particles; however, the large signal pulses they produce
make it relatively easy to detect radiation, be it alpha, beta, or gamma radiation.

11.5.1 Counting Plateau


As with proportional counters, proper operation of a G-M counter requires the appropriate voltage setting.
At too low a voltage, the detector functions in the ion-chamber or proportional regions, and generally less
efficiently than detectors designed for such operations. As previously discussed, the amplitude of signal
pulses from a G-M counter operating in region IV of the gas pulse height curve is strongly dependent upon
the space charge sheath required to terminate the Geiger discharge. Consequently, as voltage is increased
in the Geiger-Müller region, the amount of space charge required to terminate the discharge also increases.
If the operating voltage is further increased, eventually the detector is driven into a state of continuous
discharge (region V).
An operator can determine a proper operating voltage as follows. First the detector is placed in a
well-shielded or relatively radiation-free environment, and the high voltage is applied to the detector in
increasing increments. In doing so, the operator establishes the discrimination level LLD necessary to
eliminate electronic noise. Then the high voltage is reduced back to zero and a calibration source is placed
in the vicinity of the detector. Signal input pulses produced by radiation particles from a detector operating
in the ion-chamber or proportional regions are smaller than pulses produced in the G-M region and depend
on the type of incident radiation. Also, pulses produced from mixed α and β sources have a large variation
in signal amplitudes when the detector is operated in either the ion-chamber or proportional regions. As
voltage is increased beyond the proportional region, the variation in pulse amplitudes reduces and the pulse
amplitudes, although increasing with increasing voltage, converge to equal amplitudes in the G-M region.
If the signal pulse amplitudes produced by β and α particles are equal, within statistical fluctuations,
then detector operation is at the beginning of the G-M region. The LLD is set at the signal voltage produced
at the onset of the G-M region, as depicted in Fig. 11.1. Because Geiger discharges produce voltage pulses
Sec. 11.5. Radiation Measurements 413

of equal amplitudes, at any set voltage, for any type of incident ionization radiation, the LLD is mostly
ineffective at eliminating background radiations; however, the equality of the pulse amplitudes can be used
to ensure that the detector is operating in the G-M region. With a source present, the operator can then
track the count rate as a function of applied voltage, thereby producing a counting curve.
a operating operating Consider Fig. 11.8(a), where it is shown that
Pulse Height Distribution
background & (a) voltage = V voltage = V (b)
electronic noise
1 2
alpha and beta particles have significantly dif-
Energy Distribution

b ferent energy spectra. When these particles in-


a and b
a and b
particles increasing
operating particles teract in a G-M counter, the pulses they produce
voltage
are indistinguishable as shown in Fig. 11.8(b),
thereby producing a continuous pulse height
spectrum. With the LLD set to some arbi-
E LLD Output Voltage
trary level, Geiger discharges that produce volt-
(c) (d) age pulses below the LLD threshold are not
a plateau continuous recorded. The combined spectrum of pulses
Count Rate

Count Rate

counting
plateau
discharge from the α and β particles increases as the op-
continuous
discharge
b plateau erating voltage increases. Further, the increase
in signal amplitude allows some pulses to sur-
mount the LLD threshold and causes a rapid in-
V1 V2 V V crease in count rate as shown in Fig. 11.8(c). At
Figure 11.8. (a) Although the energy spectra of α and β particles higher voltages, all Geiger discharges exceed the
are different, the (b) combined signal pulses from Geiger discharges, LLD threshold and produce a counting plateau
regardless of radiation energy or particle type, are nearly indistin-
guishable. At low operating voltages V , the resulting signal volt-
as shown in Fig. 11.8(c). At higher voltages,
ages fall below the LLD. As the operating voltage is increased, the continuous discharging occurs and appears as a
signal voltages increase until most or all surpass the LLD thresh- large increase in count rate. If the operator were
old. (c) For a set LLD threshold, pulses below the LLD are not to compare the counting plateaus for separate
counted, whereas, for higher applied voltages that produce Geiger
discharges above the LLD threshold, the counts are recorded. (d) alpha and beta particle sources, both with the
Because the signal pulses are indistinguishable between α and β same LLD setting, then the counting plateaus
(and γ) particles, their counting plateaus (for separate and com- would appear at approximately the same volt-
bined sources) appear at nearly the same applied high voltages. age, as depicted in Fig. 11.8(d) and shown in
the measurements of Fig. 11.10. Typically, after the counting plateau is measured, the operator sets the
operating voltage in the center of the plateau. Note that the plateau formed by the β-particle source is
considerably flatter and wider than the plateau formed by the α-particle source, a feature not seen in a
proportional counter.
The slope of the counting plateau is determined in the same man-
high stray ner described by Eq. (10.60) and Eq. (10.61). The slope of the curve is
capacitance
caused for two main reasons [Centronic 2014]. (1) The increased voltage
Count Rate

causes the active volume of the detector to expand, thereby increasing


normal
curve
the count rate. (2) Even with a quench gas present, there remains a small
probability that residual positive ions or excited gas molecules may pro-
effect of stray
capacitance duce a spurious count, an effect that increases with voltage. The slope of
the counting plateau can also be affected by stray capacitance associated
V
Figure 11.9. Stray anode capacitance
with the detector anode (see Fig. 11.3). This anode stray capacitance,
from signal wires can cause problematic generally arising from signal wires connecting to the detector, has delete-
distortions in the counting curve. rious effects upon the detector performance [Centronic 2014], manifested
as a shortened counting plateau and increased plateau slope (see Fig. 11.9). Other effects include an increase
in dead time, shortened tube life, and spurious counts.
414 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

Figure 11.10. (left) A comparison of α- and β-particle counting plateaus from a single Geiger-
Müller counter for different α- and β-particle sources with different activities, and (right) the count
rate data normalized at 1320 volts. The LLD was kept constant for all measurements.

11.5.2 Alpha and Beta Particle Counting


Geiger-Müller counters have a thin central wire on the axis of a cylindrical tube, as depicted in Fig. 11.3. Most
Geiger-Müller counters are completely sealed, and consequently, alpha and beta particles can be blocked by
the detector wall from entering the sensitive volume of the detector. However, there are G-M tubes designed
for α and β particle detection that have thin windows to allow charged particles to enter the sensitive
gas-filled volume.
Although alpha particles typically have sufficient energy to pass through a window composed of boPET
or mica, the transport of particles through air from the source to the detector window may result in so much
energy loss they cannot pass through the window or, perhaps, not even reach the window. Consequently,
the window portion of the detector should be positioned within a centimeter or so of the suspected source
material so that alpha particles can enter the device.
It is also common for survey units to be enclosed and sealed in a plastic envelope or bag, mainly to prevent
inadvertent contamination of the delicate entrance window. If the plastic bag becomes contaminated, it
can be properly discarded and replaced with a new one. Unfortunately, such an envelope can prevent
the entrance, and detection, of alpha particles and low-energy beta particles. Consequently, detection of
alpha particles with a survey unit does run the risk of possible contamination of the detector window. Some
manufacturers have a metal guard screen secured in front of the window to reduce the possible contamination
or damage to the thin window. Plastic protection caps are also available that can be slipped over the entrance
window, thereby protecting the thin window from damage or contamination while still permitting gamma-ray
detection.
Energetic beta particles can pass through thin plastic and have manageable ranges in air. As a result,
even enclosed in a plastic bag, a G-M counter can usually be used for counting beta particles. However, there
are a few important radionuclides that emit low energy beta particles that present a detection challenge.
These include 3 H, 14 C, and 45 Ca, which have, respectively, maximum emission energies of 18.6 keV, 154
keV, and 250 keV, low enough to be absorbed by any intervening materials such as air or the detector
window, unless special precautions are exercised. For typical G-M counters with window mass thicknesses
equivalent to 30 mg cm−2 , the transmission percentage is ∼ 0%, 0.04% and 3.0% for 3 H, 14 C, and 45 Ca,
respectively.7 There are commercial detectors with thin windows formed of mica or aluminized boPet, with

7 Because it is difficult to measure low energy beta particles with a survey meter, liquid scintillation counting has become the
preferred measurement choice for low energy beta particles.
Sec. 11.5. Radiation Measurements 415

mass thicknesses of 1–2 mg cm−2 , that can be used to detect beta particles from 14 C and 45 Ca, although
tritium still remains a problem largely because of the short range of its beta particles in air. Higher energy
beta particles can enter detectors with thicker windows; hence, common G-M counters can be used to detect
beta particles with Emax > ∼ 250 keV.

11.5.3 Gamma-Ray Detection


Gamma-ray detection with G-M counters is fairly straightforward. To detector gas

reduce dead time, the gas in G-M tubes usually has pressures of less Compton
than 1 atm, and it is unlikely that a gamma ray interacts with the photoelectron electron

rarefied detection gas. Instead, x rays and gamma rays mostly inter-
act with the walls of a G-M counter to produce an energetic electron,
maximum
either through photoelectric, Compton scattering, or pair-production range tube
interactions, as shown in Fig. 11.11. If an energetic electron escapes wall
photons
into the detector gas, then it produces electron-ion pairs in the gas,
which subsequently cause a Geiger discharge.
The response of Geiger-Müller tubes to gamma-rays is dependent
upon the cathode material. From Fig. 11.12, it is evident that high
Z elements have an “over-response” to low-energy gamma rays. The Figure 11.11. Gamma-ray interactions
intrinsic efficiency of a G-M counter is defined as the number of primary in the G-M tube wall produce energetic
electrons emitted into the counter gas divided by the number of photons electrons that can enter the detector gas
and create electron-ion pairs. Electrons
incident on the detector. Hence, intrinsic efficiency includes gamma- liberated too far from the gas interface,
ray absorption and electron escape probabilities. For low energy gamma or scattered away from the gas-wall in-
rays, for which photoelectric absorption is dominant, σph ∝ Z 4 /E 3 and terface, cannot enter the detector.
large Z materials have higher absorption probabilities for gamma rays
than do small Z materials. Consequently, the response of G-M counter
to gamma rays is much higher for large Z materials than small Z materials in the low energy region and,
thus, causes the observed over response (see Fig. 11.12).
In the energy region largely dominated by Compton
scattering, the gamma-ray interaction probability is ap-
proximately proportional to Z, whereas the electron es-
cape probability is approximately proportional to Z −1 ;
hence the two probabilities more or less cancel. As a
result, the G-M counter response to gamma-rays in the
intermediate region between 500 keV and 2 MeV is rela-
tively unaffected by the Z of the cathode material. From
Fig. 11.12, it is seen that Al (Z = 13) and Bi (Z = 83)
have nearly the same response for 1 MeV gamma rays.
Although older G-M tube designs were lined with Bi or
Pb, modern detectors generally have a Cr/Fe stainless
steel alloy8 cathode, and for enhanced gamma-ray re-
sponse a Pt (Z = 80) cathode liner [Centronic 2014].
Figure 11.12. Gamma-ray detection efficiency in a Gei-
The Cr/Fe alloy can be processed to have a relatively
ger-Müller counter as a function of energy and cathode ma- high work function, thereby reducing the probability of
terial. Data from [Bradt et al. 1946, Sinclair 1956]. secondary electron emission. Further, the Cr/Fe stain-

8 446 stainless steel and is composed of 73% Fe and between 23% and 27% Cr.
416 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

less steel alloy is non-corrosive in the presence of the halogen quenching gas, while still having a reasonable
response to gamma rays at approximately 1% detection efficiency.
The response of G-M counters can be tailored by carefully
selecting cathode materials inserted into the chamber. However,
this practice is impractical for commercial sealed tubes, most of
which are manufactured with stainless steel cathodes. Instead,
instruments frequently come with an external shutter that the
Geiger Mueller Tube
operator can open or close so as to change the G-M counter
600
response to low- and high-energy gamma rays. Some commercial
500
manufacturers offer detachable field flattening filters designed for
Counter Rate (cpm)

400 special purposes, to reduce the over response to gamma rays at


300 low energies.
200 The gamma-ray counting efficiency is also a function of the in-
100
teraction location. An x-ray photograph of a Geiger-Müller tube
is shown in Fig. 11.13. The tube, manufactured from stainless
0
0 1 2 3 4 5 6 7 8 9 10 11 12 13 steel, rests inside an aluminum casing, connected to electronics
Length from Front Window (cm)
through a “C”-type connector. The actual G-M tube takes up
Figure 11.13. (top) X-ray photo of a Lud-
approximately 60% of the Al casing. Also shown in Fig. 11.13 is a
60
lum LND 723 G-M tube in its Al container. count rate profile from a collimated Co source. The count rate
The detector gas occupies about 60% of the alu- is highest near the center of the actual G-M tube, but drops off
minum casing with the remainder filled with wire near the entrance window and also near the anode feed through.
leads, connectors and resistive divider compo-
nents. (bottom) The count rate response as a Counts observed from positions beyond the G-M tube are from
collimated 60 Co gamma-ray source moves along Compton scattered gamma rays that interact with the Al casing
the container axis. and other materials surrounding the G-M tube.

11.6 Special G-M Counter Designs


Although G-M counters produce substantially similar output pulses regardless of the interacting radiation,
special design features can be implemented to improve responses to specific forms of ionizing radiation.
For instance, G-M tubes designed for alpha particle counting are outfitted with a thin mica window that
allows easy penetration of alpha particles into the chamber. Other designs are optimized for beta particle
penetration with either a thicker entrance window that blocks alpha particles or with thinned regions along
the metal tube length. Some designs may include a shutter that can be optionally rotated into place to block
beta particles while passing gamma rays (see Fig. 11.18). Such devices can be used to distinguish between
beta-particle and gamma-ray induced counts.
Detectors may also be filled with different types of counting gas, including He, Ne, Ar, Kr, and Xe for the
detection gas while CH3 or various halogens (usually Cl2 or Br2 ) are used for the quenching gas. Electron
mobility is higher in Ne gas, while gamma-ray interaction efficiency is higher in the heavier gases (Kr and
Xe). Introduction of an organic gas can also improve electron speeds and, at the same time, serve as the
quenching gas. Halogens, as already discussed, serve as a quenching gas while extending the tube life.
Detectors backfilled with Xe gas can be used for detecting low-energy gamma rays, and are often fabricated
with thin beryllium or mica entrance windows. These devices are, therefore, designed to operate with the
window-end pointing at the radiation source. To improve efficiency, these detectors have higher gas pressures
(between 600 to 800 torr) than do conventional G-M tubes. Further, the length is longer than other G-M
tubes to improve the gamma-ray absorption probability.
As already mentioned, the response to energetic gamma rays can be increased by lining the cathode with
high Z material. Detectors designed for high energy gamma-ray detection generally do not have an entrance
Sec. 11.7. Commercial G-M Counters 417

stopcock
gas inlet

guard tube
anode

cathode sleeve

Figure 11.14. (top) Diagram of a refillable cylindrical glass GM counter and (bottom) photograph
of a refillable cylindrical glass GM counter manufactured by N. Wood Counter Laboratory.

window and are usually designed for side irradiation to improve interaction efficiency. G-M counters can
be made sensitive to slow neutrons by including a Cd liner, but this modification is traditionally not done
because of intrinsic problems distinguishing between types of radiation.

11.7 Commercial G-M Counters


Commercial G-M counters of notable variety have been offered for decades. Many of the earliest G-M
counters were manufactured as glass tubes, similar to vacuum tubes. These tubes could be acquired as
refillable chambers, especially important if organic gases were used as the quenching gases. One such model
is shown in Fig. 11.14. These refillable G-M tubes allow a variety of host gases and quenching gases to
be used. Current manufacturers of G-M tubes supply numerous detector companies that install them in
portable or laboratory instruments. Although many geometries are available, there are perhaps four main
types, namely, end-window tubes, pancake detectors, thin wall beta/gamma sensitive tubes, and miniature
tubes. The variety of Geiger-Müller tubes, and the equipment in which they are installed, is much too vast
to cover in a single book chapter. More information on G-M tubes and equipment can be readily found at
internet sites for many of the larger G-M counter manufacturers.9 A few types of G-M counters are presented
here as examples.
LND Inc. is one of the largest manufacturers of gas-filled Geiger-Müller counters and has provided G-
M counters to commercial detector instrumentation companies for over 50 years, and a large variety of
configurations with different detection gases are available. Their G-M counters are often filled with Ne gas
under a mild vacuum, with a small amount of halogen added, usually Cl2 or Br2 . The use of Ne as the gas,
under slight vacuum, reduces the dead time of the detector by increasing the electron and ion mobilities and
drift speeds (see Fig. 10.10). To reduce corrosion from the halogen quenching gas, the cathode and anode
are constructed from 446 stainless steel. LND provides G-M counters to many detector manufacturers who
package them in a variety of configurations, including laboratory detectors, handheld instruments, and portal

9 For
example Centronic, LND, Ludlum, Canberra, Thermo Fisher, and Saint Gobain have data sheets, schematics, and operating
procedures available in varying detail.
418 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

Figure 11.15. Shown are two commercial portable G-M counters manufac-
tured by Ludlum Measurements, Inc. On the left is a 44-9 G-M pancake frisker
attached to a model 14C G-M meter, and on the right is a 44-7 G-M tube at-
tached to a model 2200 scaler rate meter.

monitors. An established radiation detector instrument manufacturer is Ludlum Measurements Inc., which
offers several small and large instruments outfitted with G-M detectors. For instance, a popular instrument is
the 44-9 pancake frisker hand held G-M counter used for general survey work. This instrument incorporates
a LND 7311 pancake detector and can be attached to a variety of counters and rate meters as shown in
Fig. 11.15.
Portable battery-operated G-M counters are relatively inexpensive and convenient for general survey
work. The counters usually have a rate meter with either an analog scale or a digital counter. In either case,
the device measures the rate that radiation interacts in the detector, but does not yield any information
about the dose rate at a given location because G-M counters are insensitive to energy deposition.
G-M counters notoriously overestimate exposure and dose for low-energy gamma rays if the cathode is
fabricated from moderately high atomic number materials. Most G-M counters are presently fabricated from
stainless steel, composed primarily of Fe (Z = 25) and Cr (Z = 24). Although the atomic numbers of Fe
and Cr are not considered overly large, the gamma-ray response is still exaggerated for energies below 100
keV. However, selective choice of filters placed over the sensitive portion of the G-M tube can flatten the
response by reducing the counting efficiency at low energies, a method referred to as energy compensation.
Compensated Geiger-Müller tubes have a tubular collar as part of the detector, commonly an alloy of
Sn and Pb, placed around them to flatten the response to gamma-rays at lower energies. Some filters are
available as detachable units easily added to the sensitive window of a detector, as depicted in Fig. 11.16,
while other detector probes have a rotatable filter as part of the probe unit. Shown in Fig. 11.17 are
gamma-ray sensitivity response curves to a Ludlum standard 44-9 pancake G-M counter with and without
the optional detachable filters [Ludlum 2014b]. The exposure filter is composed of Sn (1 mm) and plastic
(.62 mm) inserts, while the dosimeter filter is composed of Al (0.4 mm), Sn (0.9 mm), and plastic (0.12mm)
inserts. G-M counters designed primarily for gamma-ray and beta-particle counting may have a thinned
portion of the tube that allows for beta particles to pass into the detector gas, but generally not as thin
as windows needed for alpha-particle counting. Probes with rotating shields allow beta-particle counting
Sec. 11.7. Commercial G-M Counters 419

cap filters
G-M tube container

connector

Figure 11.16. The gamma-ray response from a G-M counter can be altered
by adding filters to the detector entrance window. With a proper selection of
materials and orientation, the gamma-ray response of a G-M counter can be
reasonably constant over a wide range of photon energies.

Figure 11.17. Gamma-ray responses from a commercial Ludlum 44-9 G-M


pancake detector with and without filtration. The responses are normalized at
662 keV. The filters work to suppress the over-response to gamma rays at low
energies. Data from [Ludlum Measurements, Inc. 2014a, 2014b].

when the shield is opened, and filtered gamma-ray counting when the shield is closed. Detectors of this
sort are shown in Fig. 11.18, manufactured by Eberline10 and Ludlum. The Ludlum 44-6 and 44-38 G-M
probes come equipped with a Sn side shield that can be rotated in front of the thin G-M tube. The G-M
tube listed as the detector in Ludlum 44-6 and 44-38 probes is a LND 725, which does not come equipped
with a front window, but has a relatively thin stainless steel body designed to record counts from the side.11
The LND 725 is backfilled with Ne with a halogen quenching gas, usually Cl2 or Br2 . The capacitance
of the tube is 3 pF, with a recommended load resistance of 1 MΩ, thereby yielding a rise time constant
of 3 microseconds. When the Sn shield is rotated back, the G-M tube is exposed through open windows
along the probe body (see Fig. 11.18), thereby allowing beta-particle counting for energies above 200 keV
[Ludlum 2013a]. Shown in Fig. 11.19 is the gamma-ray response, with and without the shield, for a LND 725
G-M tube installed in a Ludlum 44-6 or Ludlum 44-38 handheld probe. The data were recorded with a few

10 Now owned by Thermo Fisher.


11 Some of the Ludlum 44-6 probes come equipped with a TGM N112 G-M tube with similar properties as the LND 725.
420 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

Pencil
Clip O-Ring
O-Ring
G-M Tube
Bottom
Base Main Body Rotating Shield
Grounding Plastic
Ring Bushing

Figure 11.18. (top) Eberline HP177 G-M beta gamma hand probes with rotating shield, showing
closed and open positions. The G-M tube was manufactured by Anton Electronics Laboratory.
(bottom) Exploded view of a Ludlum 44-6 G-M beta gamma hand probe. From [Ludlum Mea-
surements, Inc. 2013a].

Figure 11.19. Gamma-ray response from an LND 735 G-M tube


installed in commercial Ludlum 44-9 and 44-38 beta-gamma counters
with and without filtration, normalized at 662 keV. The filters work
to suppress the over-response to gamma rays at low energies. Data
from [Ludlum Measurements 2013a, 2013b].
Problems 421

gamma-ray standard check sources, namely, 241 Am, 57 Co, 133 Ba, 137 Cs, and 60 Co. Because 133 Ba and 60 Co
have multiple gamma-ray emissions, weighted averages for their emission energies were reported [Ludlum
2013a, 2013b].
Although G-M counters are used widely for portable handheld instrumentation, there are some larger
instruments that have several G-M tubes operating as a single unit. For instance, portal and contamination
monitors have multiple G-M counters installed in them. Hand and shoe monitors have multiple G-M counters
installed in hand ports and underneath a foot screen for shoe monitoring. A single instrument may have
over 20 pancake type G-M tubes, divided amongst the hand and shoe locations. Portal monitors have G-M
tubes of varying geometries arranged about a frame that surveys the entire body.

PROBLEMS
1. Consider Fig. 11.10. Why is the β-particle counting plateau for a G-M counter wider and flatter than
achieved with a proportional counter?

2. A G-M tube, which contains 0.12 atm of argon and 0.01 atm of alcohol, has a lifetime of 2 × 109 counts.
If the end of the tube life occurs when all the alcohol molecules have been dissociated, estimate the
number of alcohol molecules dissociated per discharge.

3. If the voltage applied to a G-M tube increases above that needed to achieve a full Geiger discharge, the
pulse height continues to increase. Explain.

4. What would be the effect on the starting voltage of the Geiger plateau if (a) the pressure of the fill gas
were doubled, or (b) the small concentration of the quench gas were doubled, or (c) the diameter of the
anode wire were doubled?

5. An engineer decides to test a G-M counter with Ar as the host gas without the quenching gas. Estimate
the number of electrons ejected from a cathode wall for a 5 MeV alpha particle fully absorbed in a G-M
counter. Assume M = 1000 and the photoelectric efficiency of the wall is 10−4 .

6. Consider a typical G-M tube with dimensions of D = 2.5 cm and L = 15 cm. The tube is pressurized
to 0.15 ATM with Ne gas along with 0.1% Cl2 gas. If the quenching gas does not recombine, estimate
the limiting number of counts possible with this G-M tube. If the actual number of counts observed is
1013 , what conclusions can you draw about the quenching gas?

7. While operating a G-M counter, the LLD is adjusted such that the resolving time is 220 μs. At what
count rate do resolving time losses reach 5% for this detector? Plot the resolving time losses as a function
of count rate from 0% up to 10% loss.

8. A G-M tube is used with a counting system that requires a full Geiger discharge in order to register a
count. Is the dead time of such a system better described by an extendable or nonextendable model?
Explain.

9. If a G-M counter internal wall is coated with 10 B, or is instead backfilled with 3 He or BF3 gas, it can
be made sensitive to neutrons; however, this is typically not done. Explain the disadvantage to using a
G-M tube for neutron detection.
422 Gas-Filled Detectors: Geiger-Müller Counters Chap. 11

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New York: Van Nostrand Co., 1946. SINCLAIR, W.K., “Geiger-Mueller Counters and Proportional
Counters,” in Radiation Dosimetry, G.J. Hine and G.L. Brown-
LIEBSON, S.H., “Low Voltage Self-Quenching Counters,” Phys. well, Eds., Ch. 5, 213–243, (1956).
Rev., 72, 181–182, (1947a).
SPATZ, W.D.B., “The Factors Influencing the Plateau Character-
LIEBSON, S.H., “The Discharge Mechanism of Self-Quenching istics of Self-Quenching Geiger-Mueller Counters,” Phys. Rev.,
Geiger-Mueller Counters,” Phys. Rev., 72, 602–608, (1947b). 64, 236–240, (1943).
LIEBSON, S.H. AND H. FRIEDMANN, “Self-Quenching Halogen- WERNER, S., “Die Entladungsforman im Zylindrischen Zählrohr,”
Filled Counters,” Rev. Sci. Instrum., 19, 303–306, (1948). Z. Phys., 90, 384–402, (1934a).
LUDLUM MEASUREMENTS, INC., Ludlum Model 44-6 Beta- WERNER, S., “Die Entladungsforman im Zylindrischen Zählrohr
Gamma Detector, Product Manual, 2013a. II,” Z. Phys., 92, 705–727, (1934b).
Chapter 12

Review of Solid State Physics

Nothing exists except atoms and empty space; everything else is opinion.
Democritus

12.1 Introduction
Before scintillation detectors are discussed in the next chapter and light collection devices are discussed in
Chapter 14, it is necessary to have this introductory chapter on solid state physics. Further, the information
in this chapter is also pertinent to the chapters on semiconductor radiation detectors (Chapters 15 and
16). Here many basic concepts are developed including the fundamental theory of solid state energy bands,
effective mass, density of states, mobility, resistivity, impurity doping, and compensation methods. Note
that those already familiar with basic solid state physics, including band theory and electronic properties of
materials, may safely proceed on to Chapter 13 with, perhaps, little consequence.

12.2 Solid State Physics


Proficiency in the design and fabrication of scintillation and semiconductor detectors requires an understand-
ing of basic solid state and semiconductor physics; and addressing this requirement is the purpose of the
present chapter. Here the necessary background about crystalline solid state materials is presented. The
physics reviewed here is needed for the chapters that follow.

12.2.1 Crystals and Periodic Lattices


A crystal is composed of atomic or molecular structures (the basis) arranged and repeated in a lattice
arrangement [Kittel 1966]. The basis of the system is the grouping of atoms, which may be a single atom
or may be a large molecular group of atoms. The lattice is the structure onto which the basis is projected
and repeated. Together they form a crystal structure. Figure 12.1 depicts the basis and lattice of a crystal.
When the basis is placed upon each of the lattice points, a crystal is formed. The lattice itself is a periodic
structure that can be reduced to a single unit cell which, when repeated, reproduces the entire crystal. In
other words, by simply repeating the unit cell over and over with each unit cell placed adjacent to the last,
a crystal is formed. Figure 12.2 shows two possible unit cells for the lattice, both of which are valid. Unit
cells do not have to be primitive cells, which are the smallest possible unit cell that, when repeated, forms
the crystal. In fact, unit cells are not unique and can be formed in many geometric shapes, provided that
the shapes, when stacked, again form the crystal.
The unit cell is related to the lattice in terms of basis vectors. Consider the two lattices shown in
Fig. 12.3. Then a is a basis unit vector of length a, and b is a basis unit vector of length b. An equivalent

423
424 Review of Solid State Physics Chap. 12

+
basis

lattice

crystal Unit Cells

Figure 12.1. A crystal is formed by re- Figure 12.2. Two possible unit cells for the
peating a basis over the points of a lattice. lattice shown.

point anywhere on the lattice can be found by translating the basis vectors by integers. In other words,
equivalent points in a two-dimensional lattice can be represented by

r = ha + kb , (12.1)

where h and k are positive or negative integers. As a result, the entire crystal can be reproduced by
translating the unit cell by allowing the integers h and k to assume all possible values.

Unit Cell

Unit Cell b b
b
b a
a a
a

(a) (b)
Figure 12.3. The unit cell can be defined by the unit basis vectors, a
and b with magnitudes a and b, respectively. Shown are (a) rectangular
and (b) oblique 2-dimensional lattices. Notice that the unit basis vectors
are oriented in space according to the lattice alignment points, and is not
necessarily a Cartesian system.

12.2.2 Bravais Lattice


It turns out that there are only five possible lattices for a 2-dimensional crystal. The five possibilities,
referred to as the 2-dimensional Bravais lattices, named after the man who categorized them [Bravais 1850],
are shown in Fig. 12.4. There are four crystal systems, namely the square, rectangular, oblique and hexagonal
systems. The centered rectangular is part of the rectangular system, in which an additional lattice point is
centered within the rectangle. Hence, the simple rectangle has one lattice point per unit cell (1/4 lattice
point per corner), whereas the centered rectangle has two lattice points per unit cell. However, it should be
Sec. 12.2. Solid State Physics 425

Square Rectangular
b

-1
tan (a/b)
Centered Rectangular

Oblique
Hexagonal

Figure 12.4. The 5 different 2-dimensional Bravais lattices.

pointed out that the centered rectangle can be represented as a special form of the oblique lattice, in which
the angle formed between the basis vectors is represented by tan−1 (a/b) with a and b being the magnitude
of the two different sides of the rectangle. Hence, the reduced oblique lattice has only one lattice point per
unit cell and half the volume of the centered rectangular cell.
The concept can be expanded to 3 dimensions, in which a 3-dimensional crystal can be described by

r = ha + kb + lc, (12.2)

where h, k and l are integers. As before, the entire crystal can be reproduced by translating a unit cell
by consecutively translating the basis vectors alternately in the a, b and c directions, i.e., by allowing the
integers h, k and l to assume all possible values. Although the number of possible unit cells is enormous,
there are only 14 possible point lattices for a 3-dimensional system, which are shown in Fig. 12.5. Table 12.1
lists the conditions that define the 7 different crystal systems and the 14 different three-dimensional Bravais
lattices. The angles between the basis vectors are denoted α, β and γ, in which

b•c = |b||c| cos α a•c = |a||c| cos β a•b = |a||b| cos γ. (12.3)

The cubic system has three unique lattice arrangements, the most fundamental unit being the simple
cubic. By placing a lattice point in the center of the cubic unit cell structure, the body-centered cubic unit
cell is formed. The third fundamental unit cell is formed by placing centered lattice points on the faces of the
cube, thereby producing a face-centered cubic unit cell. The simple unit cell is denoted as P (for primitive),
the body-centered as I (from the German Innenzentrierte), and the face-centered as F. Notice that some
crystal systems have a single set of faces with a lattice point, denoted as C for base-centered. However, such
an arrangement for the cubic system can be shown to produce a tetragonal P unit cell, and therefore does
not constitute a unique cubic lattice arrangement. The tetragonal system has P and I unit cells, yet does
not have unique F and C unit cells. It can be shown that a tetragonal F cell can be reoriented such that it
is actually a tetragonal I unit cell. Further, the tetragonal C cell can be reoriented such that it is actually
426 Review of Solid State Physics Chap. 12

Simple Cubic Body-Centered Cubic Face-Centered Cubic


(P) (I) (F)

Simple Tetragonal Body-Centered Tetragonal


(P) (I)

Simple Base-Centered Body-Centered Face-Centered


Orthorhombic Orthorhombic Orthorhombic Orthorhombic
(P) (C) (I) (F)

Simple Triclinic Trigonal


Base-Centered
Monoclinic (P) (R)
Monoclinic
(P) (C)

a a
a
Hexagonal
(P)

Figure 12.5. The 14 different 3-dimensional Bravais lattices.

a simple tetragonal P unit cell. The trigonal system has a single rhombohedral primitive unit cell, denoted
as R. The hexagonal unit cell can actually be shown to be composed of three primitive rhombohedral cells,
much like the 2-dimensional counterpart.

12.2.3 Miller Indices


Thus far it has been shown that a crystal is composed of a basis and a lattice. Further, there are only 14
possible Bravais lattices for 3-dimensional crystals. Shown in Fig. 12.6 is a coordinate system for a cubic
Sec. 12.2. Solid State Physics 427

Table 12.1. Conditions for the 7 crystal systems and 14 Bravais lattices.

System Dimensions and Angles Lattices in System

Cubic a=b=c P primitive


α = β = γ = 90o I body centered
F face centered

Tetragonal a=b=c P primitive


α = β = γ = 90o I body centered

Orthorhombic a=b=c P primitive


α = β = γ = 90o C base centered
I body centered
F face centered

Monoclinic a=b=c P primitive


α = γ = 90o = β C base centered

Triclinic a=b=c P primitive


α=β=γ

Trigonal a=b=c R rhombohedral primitive


120o > α = β = γ = 90o

Hexagonal a=b=c P primitive rhombohedral


α = β = 90o , γ = 120o

three-dimensional lattice. Lattice planes can be defined by Miller indices1 . To describe a single plane, the
following procedure is used:

1. Set up a coordinate system along the edges of a unit cell.


2. Note where the plane of interest intercepts the axes and record those integer values. If a plane is
parallel to the axis, then it is stated that it intercepts it at ∞. A minus sign is placed over the number
for intercepts in the negative direction.
3. Invert the intercept values and convert to the smallest set of whole numbers.
4. Enclose the numbers in curved brackets (hkl).

For example, the plane shown in Fig. 12.6 has intercepts at h = 3, k = 2, and l = 4. Inversion gives 13 , 12
and 14 . Multiplication by 12 reduces the set to the smallest whole numbers, hence the plane is identified as
the (463) plane.
Finally, the set of equivalent planes by symmetry are designated by curly brackets, {hkl}. Note that in
the cubic system that a set of planes applies to all permutations with the same indices. For instance, (100),
(010), (001), (100), (010) and (001) all belong to the {100} set of planes. This is not necessarily the case
for other crystal systems. For instance, in the tetragonal system, (100), (010), (100) and (010) all belong to
the {100} set of planes, but the (001) and the (001) planes are dissimilar to the {100} planes, and instead
belong to the set of {001} planes. Hence, extra care should be taken with non-cubic coordinate systems.
The direction vector describes a specific direction in the crystal lattice, and is found in the following
manner:

1 In1829, the system of Miller indices was introduced by W. Whewell, the Chair of Mineralogy at Cambridge University. His
successor was W.H. Miller who further developed the system, also receiving his name, and in 1839 published in his book “A
Treatise on Crystallography” [Faria 1990].
428 Review of Solid State Physics Chap. 12

1. Set the vector in the direction under investigation.


2. Compose a basis vector r by noting its projections along the coordinate axes.
3. Use a multiplier to convert to the smallest set of whole numbers.
4. Assign a direction vector, r = ha + kb + lc.
5. Enclose the numbers in square brackets, [hkl].
z Direction vectors perpendicular to lattice planes have identical
Miller indices for the three cubic crystal lattices, a condition that
c{
is not necessarily true for any of the other 11 Bravais lattices. For
example, Cartesian coordinates with axes x, y and z can be used for
a cubic lattice. The direction shown in Fig. 12.6 has projections at
h = 4, k = 6, and l = 3. The numbers are already reduced to the
(463) plane
smallest of whole numbers, so that the direction is denoted as the [463]
[463] direction
o
90 direction. As with planes, the minus sign is placed over the number
y for projections in the negative direction. The set of symmetrically
{

b
a equivalent directions are designated by triangular brackets, hkl.
{

One of the more common lattices encountered in semiconductors,


x although definitely not the only one, is the cubic lattice. Si, Ge, GaAs,
CdTe, CdZnTe, and InP are all cubic lattice materials, whereas HgI2 ,
Figure 12.6. Miller indices are used to
identify crystal planes and directions. In GaSe, and PbI2 are not. Common planes referenced when dealing
the cubic system, the crystal plane (hkl) with cubic crystals are shown in Fig. 12.8. There are occasions in
has direction [hkl] orthogonal to the plane. which planes must be described that fall between lattice planes, as
c shown in Fig. 12.9. For instance, the (200) plane falls between two
(100) planes, where the use of the numeral 2 indicates that it falls
halfway between the planes. As mentioned above, cubic lattices have
a unique feature that the [hkl] directions are orthogonal to the (hkl)
-
(1100) planes, as with the example in Fig. 12.6. This feature is a direct result
of the high symmetry along the three axes. In the cubic system the
spacing d between the atomic planes is
a3
a
d= √ , (12.4)
a2 h + k2 + l2
2

where a is the lattice constant. The cosine of the angle between two
different crystal directions for the cubic system, h1 , k1 , l1 and h2 , k2 , l2 ,
is
a1 h1 h2 + k1 k2 + l1 l2
cos θ =  2  . (12.5)
h1 + k12 + l12 h22 + k22 + l22
Figure 12.7. Coordinate system for
hexagonal crystals, showing the (1100)
Finally, not all systems are defined by only three Miller indices. The
plane. The system is typically described
with four index values. hexagonal lattice requires four Miller indices, namely hkil, in which
h, k and i are integers along the a1 , a2 and a3 axes, and l is along
the c axis, as shown in Fig. 12.7. Also shown in Fig. 12.7 is a plane that intercepts the a1 axis at 1, the a2
axis at -1, and is parallel to the a3 and c axes. Inversion and reduction to the smallest integer set of whole
numbers, the plane is found to be the (1100) plane. Because a hexagonal unit cell is really three primitive
rhombohedral cells, it is really only necessary to have three Miller indices for the hexagonal lattice; however,
the established convention remains with four.
Sec. 12.2. Solid State Physics 429

z
c
z
c (200)
y z
b
a
(100) x c
y z
b
a (220)
x c
y
z b
(110) a
x
y c
z b
a
x (222)
c
b
y
(111) a
x
b
y
a
Figure 12.9. Planes that fall between lattice
x planes can be described without reducing the
Miller indices to the lowest integer. Shown are
Figure 12.8. Common planes referred to and three examples in which the (200) plane falls
used for cubic crystals, showing the (100), (110) halfway between two (100) planes, the (220)
and (111) planes. The directions for the planes plane falls halfway between two (110) planes and
are perpendicular to the planes, namely [100], the (222) plane falls halfway between two (111)
[110] and [111], respectively. planes.

12.2.4 Reciprocal Lattice


Crystalline planes are described in what is usually referred to as reciprocal lattice space, a concept used
throughout this text. From the real lattice space, which uses unit basis vectors a, b, and c, the fundamental
reciprocal lattice vectors are [Kittel 1986]

2πb × c 2πc × a 2πa × b


a∗ = , b∗ = , and c∗ = . (12.6)
a•(b × c) a•(b × c) a•(b × c)

It is easily seen that


a∗ ⊥ b and c, b∗ ⊥ a and c, c∗ ⊥ b and a, (12.7)
and that a∗ •a = b∗ •b = c∗ •c = 2π. Notice that the denominators in Eq. (12.6) are the volume of the space-
lattice unit cell. Vectors in the real crystal lattice have dimensions of length; hence the reciprocal vectors
have dimensions of inverse length. Further, the factor of 2π adjusts the reciprocal space to be numerically and
dimensionally consistent with wave-vector space. Multiplication of each coordinate by  converts reciprocal
space into momentum space (length−1 ). From the conditions of Eq. (12.7), it is seen that

a∗ •b = a∗ •c = b∗ •a = b∗ •c = c∗ •a = c∗ •b = 0. (12.8)

The reciprocal lattice vector is


G = ha∗ + kb∗ + lc∗ (12.9)
where the reciprocal lattice vector is perpendicular to the hkl plane in real space. A reciprocal lattice can be
constructed in much the same way that a real space lattice is constructed, by simply translating each lattice
430 Review of Solid State Physics Chap. 12

point in G by having the integers h, k, and l assume all possible values. The distances between the points
in the reciprocal lattice are inversely proportional to the distances between lattice points in real space.
Suppose one wished to find the fundamental reciprocal lattice vectors for a cubic lattice. The cubic
lattice, as represented with Eq. (12.2), has all unit vectors of equal length, namely lattice constant a. For a
simple cubic lattice with lattice constant a and the use of basic Cartesian coordinates, the basis vectors are

a = aî b = aĵ and c = ak̂ . (12.10)

From Eqs. (12.6) and Eqs. (12.10), the fundamental vectors of the reciprocal lattice are found to be
2π 2π 2π
a∗ = î b∗ = ĵ c∗ = k̂ (12.11)
a a a
where î, ĵ, and k̂ are unit vectors along the x, y, and z axes. The reciprocal space is widely used in solid state
physics, and is generally referred to as k-space. The concept of reciprocal lattice space is used throughout
the text.

12.2.5 Energy Band Gap


In free space, a single atom has discrete quantized energy states for the orbital electrons. Further, the Pauli
exclusion principle states that no two electrons of an atom can have the same values for the four quantum
numbers (n, l, ml , ms ), where n is the principle number, which determines the electron’s energy, l is the
angular momentum quantum number, ml is the magnetic quantum number, and ms is the spin.
However, a solid material, such as a semiconductor crystal, is a matrix of atoms arranged in a lattice such
that the various potentials of each of the atoms affect the surrounding atoms and their associated electrons.
If two atoms, whose electrons initially have identical quantum numbers, are forced into close proximity then
something must change so that Pauli’s exclusion principle is not violated as the atoms’ electrons begin to
interact with each other. What happens is the appearance of new degenerate electron energy states. In
other words, the original quantum energy levels split such that two states appear where there was only one
before the atoms began interacting with each other.
Consider the case of a solid, in which typical atomic densities range from 1021 to 1023 atoms cm−3 . The
total number of energy states must split to accommodate the increased electron density in solids. These
degenerate energy states form bands of states in place of what were once individual states for a single atom.
These bands may overlap, they may be relatively close to each other in energy with a small energy gap
between them, or they may form with energy gaps between the bands (see Fig. 12.10). Electrons in the
bands behave almost as though they are in an energy continuum, but it is actually a quasi-continuum, in
which there is a density of available states that each of which can be occupied by an electron. The density
of states is determined by the original total number of states of the individual atoms.
The electrical conductivity of a solid is determined by many parameters such as the charge carrier mobility,
the density of free charge carriers available in a partially filled energy band, and the availability of unfilled
energy states in the partially filled band. Figure 12.11 shows simplistic band diagrams for (a) insulators, (b)
conductors, and (c) semiconductors. In Fig. 12.11(a) the valence band, which is active in chemical binding
of electrons in compounds, is filled, and the next available higher energy band is devoid of electrons. In
typical notation, the upper energy limit of the valence band is denoted EV and the lower energy limit of the
conduction band is denoted EC . The energy difference between EC and EV is a forbidden energy region,
referred to as the energy band gap and is denoted by Eg . No states exist between energies EV and EC , i.e.,
in the band gap. If the band-gap energy is sufficiently large, electrons cannot be thermally excited from
the valence band into the conduction band. Such materials are said to be insulators. Conduction occurs
only if there are empty states in the same energy band for charge carriers to occupy as they move through
Sec. 12.2. Solid State Physics 431

band of energy states


Energy

band gap

band of energy states

band gap
band of energy states

band gap

band of energy states

Atomic Spacing
Figure 12.10. As atoms are brought closer together, their allowed energy states split
into degenerate states. In a solid medium, the high atomic density causes these degen-
erate states to form quasi-continua referred to as energy bands.

EC
EC
EC
EV EV EV
EC

(a) (b) (c)


Figure 12.11. Depictions of simple band diagrams for (a) insulators, (b) conductors
and (c) semiconductors. In (b) there are two depictions for conductors, one in which
a filled valence band overlaps the conduction band, and the other in which the valence
band is full with a partially filled conduction band.
432 Review of Solid State Physics Chap. 12

the crystal. Because the valence band is completely full of charge carriers in Fig. 12.11, there are no empty
states and hence no conduction. Further, the conduction band has empty states, but no charge carriers,
hence again conduction does not take place.
In Fig. 12.11(b), there are two examples of conductors. In the first example, the valence band and
the conduction band overlap such that electrons can easily move from the filled valence band into the
partially filled conduction band without a change of energy. Hence, there are plenty of unfilled states with
an overlapping reservoir of electrons (the valence band) that can move to the conduction band, thereby
producing free conduction. In the other example, the valence band is filled, and the conduction band is
partially filled with a high density of electrons, even at low temperature. Again the conditions exist for free
conduction.
In Fig. 12.11(c), there is a band gap, similar to
Table 12.2. Constants used for Eq. (12.12). that of the insulator example, except the band gap
Semiconductor Eg0 α β is relatively small. As a result, some electrons are
Si 1.170 eV 4.73 × 10−4 636
thermally excited from the valence band into the con-
Ge 0.7437 eV 4.774 × 10 −4 235 duction band where they can freely move through the
GaAs 1.519 eV 5.405 × 10−4 204 crystal. However, the density of the electrons in the
conduction band is determined largely by the band-
gap energy and the temperature. At sufficiently low temperatures, the electrons all return to the valence
band and the material behaves as an insulator. As the temperature is increased, more and more electrons
cross the band gap into the conduction band, and the material conductivity increases. The band-gap energy
is an inverse function of temperature, with empirical dependence,
αT 2
Eg (T )  Eg0 − , (12.12)
T +β
where T is the absolute temperature, Eg0 is the band gap at absolute zero, and α and β are experimentally
determined constants. Table 12.2 shows constants reported for semiconductors Si, Ge, and GaAs [Sze, 1985].
Often the class of materials represented by Fig. 12.11(c) is separated into semiconductors and semi-
insulators, the distinction roughly defined by the band-gap energy. Typically, band-gap energies up to about
1.4 eV constitute a class of materials usually designated as semiconductors, while band-gap energies from
1.4 eV to about 5 eV are considered semi-insulators. Band gaps exceeding 5 eV form the insulator class of
materials. However, these ranges are not rigidly classified, and often semi-insulators and semiconductors are
treated as the same as done in this chapter.

12.3 Quantum Mechanics


Quantum mechanics play a key role in understanding the behavior of electrons in semiconductor materials.
An introduction to some quantum mechanics concepts and models is presented in Chapter 3. In this section
two more important quantum mechanics models are presented.

12.3.1 Potential Barriers


Quantum mechanical tunneling is a phenomenon often observed and used for the design and development
of semiconductor devices, including semiconductor radiation detectors. For instance, potential barriers form
when a metal is attached to a semiconductor surface, which can cause the contact to have undesirably high
resistance. Often, low-resistivity contacts, sometimes referred to as “ohmic contacts”, are generally made
by introducing impurity dopants on the surface along with the metal to such concentrations that barriers
forming between the metal and the semiconductor are thin, typically only a few angstroms thick. As a
result, electrons can tunnel through the potential barrier, and the effective contact resistance is reduced. By
contrast, in classical mechanics an electron that encounters the potential barrier would simply be reflected.
Sec. 12.3. Quantum Mechanics 433

U(x) Depicted in Figure 12.12 is a potential barrier of height U0 and


width a. To find a solution for transmittance of electrons, with en-
I II III ergy E less than U0 , through the potential barrier, three regions are
U0
defined: in region I (x < 0) U (x) = 0, in region II (0 < x < a)
U (x) = U0 , and in region III (x > a) U (x) = 0.2
E
From Schrödinger’s time independent wave equation, Eq. (3.33),
namely,
0 a d2 ψ 2me
+ 2 (E − U0 )ψ = 0, (12.13)
dx2 
Figure 12.12. Square potential bar-
rier in which the particle energy is less the general solutions for the three regions can be written in the form
than the barrier height. In classical
mechanics, such particles would be re- ψ1 (x) = Aeikx +Be−ikx , ψ2 (x) = Ce−φx +Deφx, and ψ3 (x) = F eikx ,
flected by the barrier.
(12.14)
where
2me E 2me
k2 = and φ2 = (U0 − E). (12.15)
2 2
The wave function in region I represents a wave traveling in the positive x direction and a reflected wave
traveling in the −x direction. In region II, reflections occur at the boundaries such that waves also travel
in both directions. In region III, it can be assumed that waves travel only in the positive x direction after
passing beyond the barrier. From the boundary condition at x = 0, namely, ψ1 (0) = ψ2 (0), it is found that

A + B = C + D. (12.16)

The boundary condition ψ2 (a) = ψ3 (a) gives

Ce−φa + Deφa = F eika . (12.17)

The boundary condition


dψ1 dψ2
(0) = (0)
dx dx
yields
ik(A − B) = φ(D − C), (12.18)
and the boundary condition
dψ2 dψ3
(a) = (a)
dx dx
gives
φ(Deφa − Ce−φa ) = ikF eika . (12.19)
Now seek a relation between A and F . Towards this end, divide Eq. (12.18) by ik and add the result to
Eq. (12.16) to yield    
φ φ
2A = C 1 − +D 1+ . (12.20)
ik ik

2 Strictly
speaking this problem should be treated with the time-dependent Schrödinger equation with the particle represented
as a wave packet moving along the x axis. But it is also possible to solve this problem as a time-independent one, by imagining
that, instead of a single particle, there is a continuous stream of particles moving towards the barrier, some of which are
reflected and the rest transmitted through the barrier.
434 Review of Solid State Physics Chap. 12

Now add and subtract Eq. (12.19) with Eq. (12.17) to obtain
   
ik ik
2Deφa = F eika 1 + and 2Ce−φa = F eika 1 − . (12.21)
φ φ

Substitute Eqs. (12.21) into Eq. (12.20) to obtain the following relationship between A and F
      
φ ik φa φ ik −φa
4A = F e ika
1− 1− e + 1+ 1+ e . (12.22)
ik φ ik φ

The above relationship is important because A defines the amplitude of the initial electron wave striking
the barrier and F defines the portion of the wave that tunnels through the barrier. By finding the ratio of
the fluxes defined by F and A, the transmission coefficient T can be determined. With a small amount of
algebra, Eq. (12.22) becomes
 
F eika 2 −φa
4A = (2ikφ + k − φ )e + (2ikφ − k + φ )e
2 2 φa 2
, (12.23)
ikφ

which can be rewritten as


 
F eika −φa −φa
4A = φa
2ikφ(e + e ) − (φ − k )(e − e
2 2 φa
) . (12.24)
ikφ

Equation (12.24) can be written in terms of hyperbolic sines and cosines such that
 
F eika
2A = 2ikφcosh(φa) − (φ2 − k 2 )sinh(φa) . (12.25)
ikφ

The magnitude of A is easily found from Eq. (12.25) to be


 
|F |2
|A| = 2 2 4k φ cosh (φa) − (φ − k ) sinh (φa) .
2 2 2 2 2 2 2 2
(12.26)
4k φ

Because |ψ(x)ψ ∗ (x)| dx is the probability of finding a particle in dx about x, the probability of finding
an electron in region I is |Aeikx A∗ e−ikx | dx = |A|2 dx, i.e., independent of position. Likewise the reflected
wave in region I Beikx and the transmitted wave in region III F eikx are also independent of position in their
respective regions. Because the electrons in the incident beam must be conserved, |A|2 = |B|2 + |F |2 or

|B|2 |F |2
1= + ≡ R + T, (12.27)
|A|2 |A|2

where R and T are the reflection and transmission probabilities or coefficients.


From Eq. (12.26)
|F |2 4k 2 φ2
T = =  . (12.28)
|A|2
4k φ cosh (φa) − (φ − k ) sinh (φa)
2 2 2 2 2 2 2
Sec. 12.3. Quantum Mechanics 435

With the identity that cosh2 (φa) − sinh2 (φa) = 1, this result reduces to

1 (k 2 + φ2 )2 sinh2 (φa)
=1+ . (12.29)
T 4k 2 φ2

Finally, the definitions of k and φ are substituted into Eq. (12.29) to yield
*  +
1 U02 2 2me (U0 − E)
=1+ sinh a . (12.30)
T 4E(U0 − E) 2

It should be obvious to the reader that the reflection probability is simply

R = 1 − T. (12.31)

From Eq. (12.30), it can be observed that the transmission coefficient approaches unity as the electron energy
approaches U0 .

Example 12.1:
For the potential barrier diagram of Fig. 12.12, suppose the following properties exist: U0 = 30 eV,
a = 0.5 Å, and E = 5 eV (for an applied voltage V0 of 5 volts). Under such conditions, how many electrons
strike the barrier per second to produce a tunneling current of 5 mA?

Solution:
Use the substitution me = 511 keV where E/c2 = m, and from Eq. (12.30),

1 (30 eV)2
=1+ ×
T 4(5 eV)(30 eV − 5 eV)
⎛ < ⎞
2(5.11 × 105 eV)(30 eV − 5 eV)
sinh2 ⎝(0.5 × 10−10 m) ⎠
(2.998 × 108 m s−1 )2 (6.582 × 10−16 eV s)2
 
= 1 + (1.8)sinh2 (0.5 × 10−10 m)(2.56 × 1010 m−1 ) = 5.965

It is found that T = 0.1676. At 5 mA, the number passing through the barrier per second is

5 × 10−3 A
nb = = 3.13 × 1016 electrons s−1 .
1.6 × 10−19 C/electron

The number of electrons ns striking the potential barrier per second is simply the number tunneling through
the barrier per second divided by T and here is found to be

(3.13 × 1016 e− s−1 )


ns = = 1.865 × 1017 electrons s−1 .
(0.1676)

Note that potential barriers found in nature are typically not square functions, hence alternative methods
to determine the transmission coefficient T are needed. One such method employs the Wentzel-Kramers-
Brillouin (WKB) approximation, the details of which can be found in the literature [Gasiorowicz 1974].
436 Review of Solid State Physics Chap. 12

12.3.2 Kronig-Penney Model


The electrons surrounding the atoms in a crystal can be thought of as confined in a series of identical
potential wells. The functions describing the individual atomic potential wells and the electron confinement
are generally quite complex. However, insight about the effect on electrons produced by a periodic series
of potentials can be obtained with the idealized assumption that the potentials are a series of square well
functions. The resulting quantum mechanical model is referred to as the Kronig-Penney model, and it is
fundamental to understanding the behavior of electrons in a semiconductor [Kronig and Penney 1931].
Figure 12.13 shows a one-dimensional infinite series of potential rectangular wells of width a and separated
by barriers of width b. Therefore the potential is a one-dimensional periodic function such that U (n(a+b)) =
U (x) where n is an integer. It is assumed that the crystal extends to ±∞; hence one need not be concerned
about effects at the termination of the periodicity at the edge of the crystal. Although such a description of
the potential an electron experiences in a crystal may strike the reader as unrealistic, it does provide a model
for the development of important concepts fundamental to solid state physics, such as crystal momentum
and carrier effective mass. These concepts are introduced in the next section.

U(x)

Uo

-b 0 a b+a
Figure 12.13. The Kronig-Penney model uses a series of rectangular wells
to represent the periodicity of the atomic potentials in a crystalline solid.
The potential is periodic, i.e., U (x + a + b) = U (x).

It seems reasonable that the wave function describing an electron in the potential of Fig. 12.13 should
also be periodic with the period of the crystal T = a + b. Indeed, in 1928 Felix Bloch showed that the energy
wave function must have the form
ψk (x) = uk (x)eikx , (12.32)
where the amplitude uk (x) also is periodic such that uk (x) = uk (x + T ) and where k is the wavenumber
defined as
2nπ
k= , n = 0, 1, 2, ... . (12.33)
a+b
The one-dimensional Schrödinger wave equation is used to describe an electron of mass me in the potential
of Fig. 12.13
2 d2 ψ(x)
− + U (x)ψ(x) = Eψ(x). (12.34)
2me dx2
Here E is the energy eigenvalue (a positive quantity < Uo ). The solution for 0 < x < a when U (x) = 0
(dropping the subscript k for the moment) is
ψ(x) = Aeigx + Be−igx , (12.35)
in which A and B are arbitrary constants to be found later from the boundary conditions. This solution is
the sum of two plane waves, one traveling to the right and the other to the left and has energy
E = 2 g 2 /2me . (12.36)
Sec. 12.3. Quantum Mechanics 437

Within the potential barrier, −b < x < 0, the solution of Eq. (12.34) is

ψ(x) = Ceγx + De−γx , (12.37)

where the positive real number γ 2 = 2me (Uo − E)/2 . Again C and D are constants to be found from
boundary conditions.
Because the wave function must have the Bloch form of Eq. (12.32), the solution ψ(x) for x ∈ (a, a + b)
must be related to the solution for x ∈ (−b, 0) by

ψ(a < x < a + b) = ψ(−b < x < 0)eik(a+b) . (12.38)

From this constraint the wavenumber k is determined and used as an index to the wave function.
The constants A, B, C, and D are chosen to make ψ and dψ/dx continuous at x = 0 and x = a. Thus
at x = 0

A+B =C +D (12.39)
ig(A − B) = γ(C − D) (12.40)

At x = a with the use of Eq. (12.38) to express ψ(a) in terms of ψ(−b), the boundary conditions require

Aeiga + Be−iga = (Ce− γb + Deγb )eik(a+b) (12.41)


ig(Aeiga − Be−iga = γ(Ce− γb − Deγb )eik(a+b) . (12.42)

For the four homogeneous equations for A, B, C, and D to have a non-trivial solution the coefficient matrix
for the four constants must vanish. After much algebra, it is found that the determinant vanishes only if

γ 2 − g2
sinh γb sin ga + cosh γb cos ga = cos k(a + b). (12.43)
2γg
Because the large potential around a nucleus is located very near the nucleus, i.e., b  a, the above result
can be simplified by approximating the potential as a periodic delta function. Thus let b → 0 and Uo → ∞
such that P ≡ γ 2 ab/2 remains a finite positive quantity [Kittel 1986]. Thus, in this approximation γ >> g,
γb << 1, and sinh γb  γb. Then Eq. (12.43) reduces to

P
sin ga + cos ga = cos ka. (12.44)
ga

Constraints to the solutions of Eq. (12.44) can be inferred from Fig. 12.14 for different values of P , in
which the left-hand side of Eq. (12.44) is plotted versus ga. Because the right-hand side of Eq. (12.44) is
bounded between ±1, it is apparent that a solution can exist for the Kronig-Penney model only for those
values of ga for which the left-hand side of Eq. (12.44) also is between ± 1. For all other regions of ga,
there are no solutions, and energy gaps appear between the regions that have solutions. This situation is
analogous to the expected effect of a periodic potential upon electrons in a solid, in which bands of allowed
energy states form, and regions also appear in which states are not allowed.
From Eq. (12.44) an allowed value of ga on the left-hand side produces a corresponding value of ka from
the right-hand side. Because k ∝ 1/λ, where λ is the wavelength of the periodic wave function, then, from
de Broglie’s relation p = h/λ between a particles momentum p and its wave length, it is seen that k is
proportional to the electron’s momentum. Likewise, from the definition of g in Eq. (12.36), (ga)2 represents
the allowed electron energies multiplied by a constant value, 2me a2 /2 . Therefore, plotting (ga)2 against ka
438 Review of Solid State Physics Chap. 12

Figure 12.15. Depiction of energy bands from the Kronig-


Penney model, showing the relationship between P, (ga)2 , and
Figure 12.14. Solutions to the Kronig-Penney model for dif- ka. Both axes are dimensionless with ka proportional to the
ferent values of P . Both axes are dimensionless. electron’s energy and (ga)2 proportional to its momentum.

produces a dimensionless energy-momentum diagram. Figure 12.15 shows the results for various values of
P for the first three regions of ka where solutions to Eq. (12.44) exist. From this figure, several important
features can be seen. Values of ka equal to multiples of π bound momentum regions in which the allowed
energies are smoothly continuous. Further, a discontinuity occurs at these boundaries in k-space, for which
gaps between the allowed energy bands appear. Notice also that as P increases, the range of the allowed
solutions of (ga)2 (or energies) in the band regions decreases. Lastly, this diagram, usually referred to as
an E-k diagram, shows that the allowed energies vary from the free electron model,3 although the basic
parabolic shape is still observed.

12.4 Semiconductor Physics


Thus far, the theory developed in the preceding sections applies in general to solid-state crystalline material.
Yet, it is the subset of solid-state materials, usually identified as semiconductors, that is generally associated
with solid-state radiation detectors. The result for the Kronig-Penney model can be used to understand
many concepts in semiconductor physics.

12.4.1 Brillouin Zones


Because of the symmetry in ka of the one-dimensional Kronig-Penney model, Fig. 12.15 can be mirrored
upon itself to produce the diagram of Fig. 12.16. The center zone is bounded by −π and +π, and it has a
continuum of allowed energy states. This first zone of allowed energies is referred to as the first Brillouin
zone in one dimension. The next Brillouin zone is defined by the regions bound between −2π and −π and

3 For a free non-relativistic electron, it can be shown that (ga)2 = (ka)2 .


Sec. 12.4. Semiconductor Physics 439

also between +π and +2π. The third Brillouin zone is bounded by −3π and −2π and also between +2π
and +3π, and so on. The total width in k-space is identical for the 1st, 2nd, and 3rd Brillouin zones and
all higher Brillouin zones [Brillouin 1953]. At the boundaries of each Brillouin zone is a discontinuity at
which an energy gap, or band gap, appears. Hence, Brillouin zones are defined as regions within which
a continuum, or more correctly a quasi-continuum, of energy states appear and terminate at the k-space
boundaries where the energy gaps appear.

Figure 12.16. Energy band formation and Brillouin zones Figure 12.17. Reduced zone diagram, showing the allowed
from the Kronig-Penney model for different values of P . energy bands and forbidden bands for several values of P .

Because one-dimensional Brillouin zones (BZ) all have the same total width in k-space, it is usual to
represent Fig. 12.2 in reduced form, as shown in Fig. 12.17. This type of plot is known as the reduced
E-k diagram. The plot is created by simply folding each consecutive BZ backwards into the first BZ. The
reduced zone diagram is used here to develop basic concepts about electron transport through the periodic
potential of a semiconductor. In a three-dimensional solid state crystal, atomic electron orbitals form the
energy bands and define the various BZs.

12.4.2 Effective Mass


Consider a wave packet of electrons influenced by an external force. To describe the motion of electrons
under such conditions the “group velocity” vg of the electron wave packet is often used. In general,
dx dω
vg = = , (12.45)
dt dk
where ω is the “center frequency” of the wave packet, and k is the wavenumber. The frequency is related to
energy by ω = E/ so that  
d E 1 dE
vg = = . (12.46)
dk   dk
440 Review of Solid State Physics Chap. 12

Application of force (F ) to the wave packet, such as occurs when an electric field is placed across the solid,
produces a change in energy of the electrons

dE = F dx = F vg dt, (12.47)

which can be rearranged as


1 dE 1 dE dk dk d(k)
F = = = = . (12.48)
vg dt vg dk dt dt dt
From Eq. (12.46),
dvg 1 d dE 1 d2 E dk
= = . (12.49)
dt  dt dk  dk 2 dt
Substitution of Eq. (12.48) for the force into the above result yields
 
dvg 1 d2 E d(k) 1 d2 E
= 2 2 = F. (12.50)
dt  dk dt 2 dk 2

Finally, Newton’s classical relationship F = ma is used to define an “effective mass” m∗ for the electrons as
 −1
dvg 1 d2 E dvg
F = m∗e = , (12.51)
dt 2 dk 2 dt

which, upon rearrangement, gives the electron’s effective mass as


 −1
1 d2 E
m∗e = . (12.52)
2 dk 2

This result, of course, does not imply the


electron’s physical mass has somehow changed,
but rather that the periodic potential defined by
E and k has changed the influence of an exter-
nal force upon the electron from that expected
upon a free electron. Often the effective mass
for electrons in a semiconductor is quoted as a
fraction of me , the rest mass of a free electron.
A few important concepts can be observed
from Eq. (12.52). In order to do so, the result
for the lowest energy band in the Kronig-Penney
model is used with P = 9π/2. In Fig. 12.18,
allowed energies E of the lowest band, dE/dk,
and d2 E/dk 2 are shown as a function of k. Be-
cause the effective mass varies inversely with
d2 E/dk 2 , it is observed that the effective mass
can be negative whenever the particle moves in
the opposite direction to that expected for the
Figure 12.18. The expected values for E, dE/dk, and d2 E/dk 2
of the lowest energy band for the Kronig-Penney model with
applied electrical force [Pierret 1989]. This sim-
P = 9π/2. ply means that the particle behaves as though it
has the opposite polarity, or in other words, the
Sec. 12.4. Semiconductor Physics 441

electron behaves as a positively charged electron. As a result, the electron moves in the opposite direction
of the applied electrical force. It is also observed that the largest magnitude of d2 E/dk 2 occurs in k-space
at the top and bottom of the energy band, so that the smallest effective mass occurs at the points of highest
curvature with respect to k of the energy band. From Fig. 12.19, in which results for the lowest energy band
for different values of P are shown, it is seen that the effective mass decreases as the energy band curvature
increases.
The bands, as depicted in Fig. 12.20, are
formed from allowed energy states, although the
available energy states may not be filled. The
lowest band formed is filled with tightly bound
electrons which typically do not share in the
chemical bonding process (except for the atoms
with very low Z numbers). At higher energies,
the band that actively takes part in chemical
binding is referred to as the valence band. Above
the valence band are various partially filled and
empty energy bands. The energy gap between
the valence band and the next band up, referred
to as the conduction band, determines, to a large
degree, the electronic properties of the solid.
For instance, overlapping valence and conduc-
tion bands generally form in a conductive ma-
terial, such as Cu. Those materials with small
band-gap energies between the valence and con-
duction bands, typically no greater than 1.6
eV, generally form a class of materials regarded
as semiconductors, such as Ge, Si, and GaAs.
Larger band gaps, ranging from approximately
1.6 eV to 5 eV compose a class of materials of- Figure 12.19. E and d2 E/dk 2 for the lowest energy band in
ten regarded as semi-insulators, which would in- the Kronig-Penney model for different values of P . Notice that
the largest absolute values of d2 E/dk 2 occur in k space at the
clude CdTe and SiC. Materials with band gaps top and bottom of the energy bands.
above 5 eV behave as insulators at room tem-
perature.
Figure 12.20 depicts a material in which the tightly bound band is filled, the valence band is partially
empty, the lower conduction band is partially filled, and the upper conduction band is completely empty.
Those electrons populating the upper portions of the bands have negative effective masses, and those elec-
trons populating the lower portions of the energy bands have positive effective masses. Under equilibrium
conditions, the electrons in the bands are evenly distributed over k-space such that their net velocities add up
to zero. This must be the case because no net current should flow from a simple solid block of semiconductor
suspended in space.
Suppose electrical contacts are placed upon the semiconductor block and a voltage is applied. Completely
filled bands do not contribute to conduction because there are no empty states in the band for electrons
to move into. Conversely, completely empty bands do not contribute to conduction because there are no
electrons available. However, for partially filled bands, the force offsets the equilibrium condition so that
electrons are displaced in k-space, as depicted in Fig. 12.21. The importance of the effective-mass concept
is that those electrons with positive effective masses flow in the direction of the applied electric field force,
but those electrons with negative effective masses flow in the opposite direction of the applied force.
442 Review of Solid State Physics Chap. 12

160

160 140

140 Upper
Conduction
120
Band
120 regions where
100 effective mass
regions where is positive
100 effective mass Forbidden Gap
80

E
is positive
80 region where
E

Conduction
Band 60 effective mass
region where is negative
60 effective mass
is negative 40
Forbidden Gap
40
Valence Band 20
20 Forbidden Gap
Tightly Bound 0
0 Lower Band -p/a 0 p/a
-p/a 0 p/a k
k
Figure 12.21. A force applied to the periodic
Figure 12.20. The reduced zone diagram depicts energy bands in structure, such as electric field force, displaces
one dimension. The bands may be completely filled, partially filled, the electron in k-space, thereby perturbing the
or void of electrons. equilibrium condition.

To determine the current, the total motion of electrons in all of the bands must be taken into consideration
[Pierret 1989]. Electric current from contributions in the lower conduction band can be written as
q 
Ic = − vi , (12.53)
d
i
filled

where the speed contributions from only those states in the conduction band filled with electrons are consid-
ered, and d is the width of the semiconductor block between the two contacts. Next, the current contributions
from the valence band are found as
q 
Iv = − vi , (12.54)
d
i
filled

where, again, the speed contributions from only those states in the valence band filled with electrons are used.
The summation of currents for the valence band can be difficult because the electrons have both positive
and negative effective mass. As a result, positive and negative velocities must also be taken into account.
This situation can be greatly simplified by introducing a few approximations. First, note that electrons
in the conduction band congregate at the bottom of the band, as occurs in semiconductors operating at
ambient temperatures. It can also be assumed that all of the electrons have positive effective mass. To
simplify further, it is apparent from Fig. 12.19 that the effective mass, inversely proportional to d2 E/dk 2 ,
is fairly constant near the top and bottom of the energy bands. Hence, those electrons in the conduction
band are assumed to have an average constant value for their effective masses. As a result, the evaluation of
Sec. 12.4. Semiconductor Physics 443

Eq. (12.53) requires knowledge only of the number of filled states in the conduction band and the average
effective mass at the bottom of the band.
Evaluation of the current from electrons in the valence band
is slightly more complicated, but the same assumptions used for 160
the conduction band electrons apply. Here it is assumed that
the empty states are all at the top of the band where electrons 140
would have negative effective mass. Again, it is assumed that the
effective mass is fairly constant at the top of the band, and that 120
an average effective mass can be used to describe the transport
of electrons. Because there is an offset of filled states in k-space, 100
where more positive effective mass states are filled than negative electrons
effective mass states, the net electron motion is from electrons 80

E
moving in the direction of the electric force. That net flow of
electrons is simply the difference between the total density of 60 holes
allowed valence band states and the number of valence band
filled states. Thus, 40
q q  q 
Iv = vi − vi = vi . (12.55) 20
d d d
i i i
all filled empty
0
which depends only on the number of empty states, all of which -p/a 0 p/a
are assumed to be in the negative effective mass region of the va- k
lence band. In other words, the number of unfilled states deter-
Figure 12.22. The valence band can be thought
mine the net number of positive effective mass electrons adding of as having “positive” charge carriers referred to
to the conduction mechanism. Because the missing electrons at as “holes” that occupy the empty states. By so
the top of the valence band would have an average negative ef- doing, the motion of the valence band electrons
fective mass, the concept of a hole is introduced. A hole is an can be replaced with a simple approximation in
which only the motion of holes is considered.
empty state that behaves like a positively charged particle in the
valence band, and mimics the situation in which the valence band is partially filled with positively charged
holes that travel in the opposite direction of the negatively charged electrons, as depicted in Fig. 12.22. As
a result, the evaluation of Eq. (12.55) requires knowledge of only the number of empty states in the valence
band and the average effective mass at the top of the band.
The conduction band of cubic semiconductors has three minima, although in some cases all three may not
be prevalent. Second, the band gap refers to the energy difference between the lowest point of the conduction
band and the highest point of the valence bands. In Fig. 12.23(a), the lowest point in the conduction band
is in the [111] direction (the L valley), and is not directly above the highest point of the valence band in
k-space. Off-centered band gaps are referred to as indirect band gaps. Semiconductors with the Γ valley
being the lowest in the conduction band are referred to as having direct band gaps because the lowest electron
energy is directly across from the highest energy of the valence bands. Third, it should be noted that three
valence bands form at Γ. Recall that the effective mass in a band decreases as the curvature of the band
increases, hence the effective masses for holes in the two upper valence bands are different. The band with
narrow curvature is the light hole band, and the band with the wider curvature is the heavy hole band. The
third and lower band is the split-off band, and is usually completely filled with electrons, hence has no holes.
Typically, the split-off band’s effect on free carrier densities is regarded as negligible and is largely ignored
in calculations.
So far the discussion has been limited to the one-dimensional case, in which regions of con-
tinuous energy in reciprocal space, or k-space, were defined by boundaries of 2π/a. A graphical
444 Review of Solid State Physics Chap. 12

E E

Eg Eg

heavy hole band heavy hole band

light hole band light hole band

split-off split-off
band band

L (111) G (000) X (100) L (111) G (000) X (100)


[111] direction [100] direction [111] direction [100] direction
Reduced Wave Vector (k) Reduced Wave Vector (k)

(a) (b)

Figure 12.23. Cubic crystals typically have three conduction band minima and three valence
band maxima. The conduction band minima are displaced in momentum space. Shown in (a) is
an indirect band-gap semiconductor and in (b) a direct band gap semiconductor.

method to develop Brillouin zones from a 2-dimensional (2D) reciprocal lattice is performed as
follows. Consider the square lattice depicted in Fig. 12.24. Choose a lattice point, depicted
here as the white point in the center. To find the first Brillouin zone, draw straight lines from this
point to the closest lattice points, indicated here by the numeral 1. These
4 3 4 lines are now bisected by perpendicular lines, shown as dotted lines, and
the zone confined in these boundaries is the first Brillouin zone, shown
4 2 1 2 4 as the white area. These bisecting dotted lines define Bragg planes. The
second Brillouin zone is found by drawing straight lines from the center
to the set of next closest lattice points, indicated here with the numeral
3 1 1 3 2. These lines are now bisected with perpendicular dotted lines, and the
regions confined by these new dotted lines and the previous dotted lines
define the second Brillouin zone, shown as the gray area. This procedure
is continued for higher order Brillouin zones.
4 2 1 2 4
These Brillouin zones in two dimensions can also be determined from
the reciprocal lattice vector [McKelvey 1966]
4 3 4
|G|2 + 2k•G = 0, (12.56)
Figure 12.24. Method of develop-
ing Brillouin zones from a 2D recipro-
cal lattice, in this case a square lattice. where G is 2π multiplied by the reciprocal lattice vector. Hence, in two
The first two Brillouin zones are shown dimensions, for a square lattice with lattice constant (spacing) of a, the
for the reciprocal lattice. reciprocal lattice is also a square lattice with lattice spacing of 1/a. Hence
it is found that [Kittel 1986],


G= (n1 x̂ + n2 ŷ), (12.57)
a
Sec. 12.4. Semiconductor Physics 445

where n1 and n2 are ± integer values and x̂ and ŷ are unit vectors in the kx and ky directions. From
Eq. (12.56) and (12.57),
π
− (n21 + n22 ) = kx n1 + ky n2 , (12.58)
a
which produces a family of straight lines in two-dimensional k-space where kx and ky are the axes, the
boundaries at which Bragg reflection occurs. The intercepts are

π (n21 + n22 )
kx intercepts = − ,
a n1
π (n21 + n22 )
ky intercepts = − .
a n2

Take the first case, in which n1 = 0, n2 = ±1 and


n1 = ±1, n2 = 0. The resulting lines are defined as the ky
boundaries at kx = ± a , ky = 0 and ky = ± a , kx =
π π

0, thereby forming a square in two-dimensional k-space 3p


a
(see Fig. 12.25). This is the first Brillouin zone. The
2p
second Brillouin zone is found by setting n1 = ±1, n2 = a

±1, producing the four lines described by kx ±ky = 2π/a


and kx ± ky = −2π/a. The reader should notice, just as p
a
with the one-dimensional Brillouin zones in which the
total length in k-space was always the same, that the -kx kx
total area of the 1st BZ is the equal to the total area 3p 2p - p p 2p 3p
-a -a a a a a
of the 2nd BZ. As with the 1-D BZ cases, the 2-D BZs
can also be folded back into the first BZ, as shown in
- pa
Fig. 12.26. The third Brillouin zone is found by setting
n1 = 0, n2 = ±2 and n1 = ±2, n2 = 0, which forms the
- 2ap
large square with boundaries of ±2π/a = kx , ky shown in 1st BZ
Fig. 12.25. Clearly the square formed has more area than 3p
-a 2nd BZ
the first two constructions, which cannot be. Fact is,
-ky 3rd BZ
there are more boundaries at which Bragg scattering can
occur. Hence, to complete the construction of the third
Brillouin zone, draw a vertical line from 0 to ky = 2π. Figure 12.25. Formation of 2D Brillouin zones, showing
Rotate the line clockwise and note where the line crosses the 1st, 2nd, and 3rd zones for a square lattice.
the next construction lines outside the 2nd BZ, which traces out the third zone. The same procedure is used
to form each consecutive BZ. The 2D Brillouin zones form regions of continuous allowed energies, and there
are gaps in the allowed energies at the boundaries, much like the result found with 1-D Brillouin zones.
These findings can now be extrapolated into three dimensions. The 3D Brillouin zones are volumes in
reciprocal (k) space, the boundaries of which satisfy the Bragg diffraction condition. As before, each Brillouin
zone has the same k-space volume as the 1st Brillouin zone. Using the example for the 2D square, the 1st
Brillouin zone for the simple cubic lattice is easily shown to be a cube. The Brillouin zones for the FCC and
the BCC lattices are quite different, and are formed in k-space by finding r for the closest lattice points,
and then finding the reciprocal lattice vectors so as to find G. The first Brillouin zone of a BCC lattice is
a rhombic dodecahedron, as can best be described, and the first Brillouin zone for the FCC lattice, which
are generally of most concern, is a tetrakaidecahedron, which is a 14-faced polyhedron (see Fig. 12.27). The
14 faces consist of 6 planes with normal vectors belonging to the 100 directions, and 8 planes with normal
vectors belonging to the 111 directions. The formation of the allowed energies and bands is different for
446 Review of Solid State Physics Chap. 12

ky

kz
3p
a

2p 2nd BZ folds back


a
into 1st BZ -
[111]

p
a
L G
-kx kx
p [010]
- 3ap - 2ap - pa a
2p
a 3p
a
ky
kx
- pa
X
1st BZ

3rd BZ folds back - 2ap 2nd BZ Figure 12.27. The 1st Brillouin zone of the FCC lat-
tice.
into 2nd BZ and then 3rd BZ
into 1st BZ - 3ap
-ky

Figure 12.26. As with 1D Brillouin zones, the 2D Brillouin


zones each have the same area in k-space, and all can be folded
back into the 1st zone.

the [100] direction than for the [111] direction, most obviously, and from results of the previous sections on
the band formation with the Kronig-Penney model, because the distance in k-space to the BZ boundary in
the [100] direction, termed X, is not the same as the distance in k space to the BZ boundary in the [111]
direction, termed L. Typically, the band diagram for FCC crystals in k space is depicted with the bands
formed in the [100] direction to the BZ boundary and the [111] direction to the BZ boundary.
Figure 12.28 depicts a typical FCC E-k diagram showing the energy bands folded back into the 1st
Brillouin zone. Only the valence bands and the first conduction band are depicted in the diagram (although
other bands may be included as well). The band gap depicted in Fig. 12.28 is indirect, displaced along the
[111] direction.
Within the first BZ (see Fig. 12.27) for a FCC semiconductor are regions of constant energy. The regions
can be depicted as constant energy surfaces. Refer back to Fig. 12.28 and notice again that there are three
minima in the conduction band. Free electron carriers accumulate at the lowest energy in one of these bands
such that they occupy energies that are quasi-continuous and bound within a region of energy defined by
the band curvature. If the Γ valley is the lowest conduction band minima, then the band gap is direct, and
electrons need only have an increase in energy to move from the valence bands up to the conduction band,
and do not need to change momentum. However, if either the L or X valleys are the lowest conduction
band minima, the band gap is indirect, and electrons must both increase in energy and have a change in
momentum. The energy bands depicted in Fig. 12.28 are three-dimensional, so that the energy surface within
which the electrons are confined is simply the band curvature rotated about the orientation axis, i.e., about
[111] for the L valley, and about [100] for the X valley, and about the zone center for the Γ valley. In Chapter
16, modeled results are shown as reported from the literature for several semiconductor energy bands.
From the Γ-valley conduction band depicted in Fig. 12.28, consider a two-dimensional crystal, where the
energy is shown as a function of wave vectors kx and ky projected along the 100 directions, as shown in
Sec. 12.4. Semiconductor Physics 447

Eg
heavy hole band

light hole band

split-off band

L ( 12 12 12) G (000) X (100)


[111] direction [100] direction

Reduced Wave Vector (k)


Figure 12.28. A typical E-k diagram for an FCC semiconductor crystal.

Fig. 12.29. Allowed energies are available provided that E > EC . A constant energy, denoted as E1 for this
example, can be depicted as an ellipse around the paraboloid surface. Hence, an ellipse with constant energy
around the periphery is described by
E1 − EC = Akx2 + Bky2 , (12.59)
where the intercept points along the axes can be identified by,

E1 − EC
kx = ± , ky = 0, (12.60)
A

E1 − EC
ky = ± , kx = 0, (12.61)
B
In the case of Fig. 12.29, the ellipse is centered about zone center, meaning that through symmetry the
parabolic energy band is identical in the ±kx and ±ky directions. Consequently, A = B, and Eq. (12.59)
reduces to the formula for a circle.
If the ellipse is displaced along an axis, as with an indirect band gap (e.g., the X valley in Fig. 12.28),
depicted in Fig. 12.30(a) by ky1 in the [01̄0] direction, the constant energy ellipse can now be described by
E1 − EC = Akx2 + B(ky + ky1 )2 , (12.62)
where the intercept points along the axes can be identified by,

E1 − EC
kx = ± , ky = 0, (12.63)
A

E1 − EC
ky = ± − ky1 , kx = 0. (12.64)
B
448 Review of Solid State Physics Chap. 12

E
2 2 constant
E1 - Ec = Akx + Bky E1 energy
ellipse

E1
-
[100]

Ec
-
[010] [010]
0 ky
E1 - Ec
E1 - Ec B
[100] kx A

Figure 12.29. Depiction of a constant energy ellipse with energy E1 − EC


centered at kx = ky = 0.

However, because the energy band minimum is no longer at zone center, the symmetry between the kx and
ky directions is lost. Hence, one can expect symmetry about zone center along the ±ky directions, finding
another energy band minimum at +ky1 . Also, the energy bands along ±kx directions are symmetric about
the location −ky1 (and also +ky1 ), but not equal to the ky bands, as depicted in Fig. 12.30(b). Here, A = B,
and the constant energy is depicted by an ellipse. There is a natural consequence to this discovery. Recall
from Eq. (12.52) that the effective mass m∗e is a strong function of the energy band curvature. Because the
curvature at the energy minimum is different in the kx and ky directions, the electron effective masses are
also different. Traditionally, the effective mass along the displaced axis (ky in the example) is called the

E
2
E1 - Ec = Akx + B(ky+ ky1)
2 constant
E1 energy
ellipse
E
E1 along kx along ky
-
[100]
E1 - Ec - k
- E1 - Ec - ky1 y1
B B
-ky1 Ec Ec
-
[010] [010]
0 ky k kmin
E1 - Ec
A
[100] kx
(a) (b)
Figure 12.30. (a) Depiction of a constant energy ellipse with energy E1 − EC
centered at kx = 0, ky = −ky1 . (b) The curvature of the energy bands are
different in the kx and ky directions.
Sec. 12.5. Charge Transport 449

longitudinal effective mass m∗l while the effective mass in the perpendicular direction to the long axis (kx in
the example) is called the transverse effective mass m∗t .
This same concept can now be expanded to three dimensions. Choosing E to lie within the energy
ranges populated by the charge carriers in the conduction band, where EC ≤ E, the allowed k values form
the surface in k-space. Because k is three-dimensional, and providing that the energy E is close to the
conduction band edge EC , the energy of the conduction band surfaces can be approximated by

E − EC  Ak12 + Bk22 + Ck32 , (12.65)


where A, B and C are constants, and k1 , k2 , and k3 are k-space coordinates measured from the center of an
energy band minimum along the principal axis. Eq. (12.65) is the equation for an ellipsoid, meaning that
the surface of the ellipsoid in all directions is a constant value.
With cubic crystals, the energy band maxima
and minima are nearly parabolic, as was discussed kz
earlier. Also, due to symmetry and expanding on
the two-dimensional example, at least two constants
in Eq. (12.65) are equal for cubic semiconductors. [111] -
Hence, the constant energy surface for an indirect
G
band gap, where the energy minimum is displaced
X
from zone center, can be rewritten as

E − EC = Ak12 + B(k22 + k32 ) (12.66) L [010]

where A is the axis of revolution.4 Here, k1 is the lon-


gitudinal axis while k2 and k3 are transverse axes.
One can imagine spinning the ellipse of Fig. 12.30 ky
about the ky longitudinal axis to form such an ellip-
soid.
For direct band-gap cubic semiconductors, all kx
constants in Eq. (12.65) are equal so that Figure 12.31. First Brillouin zone in the FCC lattice, show-
ing ellipsoids of constant energy for the L valley.
E − EC = A(k12 + k22 + k32 ), (12.67)
which is the equation of a spherical surface. Hence, it is expected to have a single spherical constant energy
surface for direct band-gap cubic semiconductors, six ellipsoidal constant energy surfaces for cubic semicon-
ductors with the lowest band minima at X, and eight ellipsoidal constant energy surfaces for semiconductors
with the lowest band minima at L. Figures (12.31), (12.32), and (12.33) depict the first Brillouin zone
for the FCC lattice along with the constant energy ellipsoids for the lowest band minima at L, X, and Γ,
respectively.

12.5 Charge Transport


To describe the transport of charges in a semiconductor, the concept of effective mass is revisited. The
three-dimensional inverse effective mass tensor is described by
⎛ ∗ −1 ⎞
mxx m∗xy −1 m∗xz −1
1
= ⎝ m∗yx −1 m∗yy −1 m∗yz −1 ⎠ (12.68)
m∗
m∗zx −1 m∗zy −1 m∗zz −1

4 This type of ellipsoid is called a “spheroid” or “ellipsoid of revolution”.


450 Review of Solid State Physics Chap. 12

kz kz

-
[111]

G G
X

[010]
L

ky ky

kx kx
Figure 12.32. First Brillouin zone in the FCC lattice, show- Figure 12.33. First Brillouin zone in the FCC lattice, show-
ing ellipsoids of constant energy for the X valley. ing a sphere of constant energy for the Γ valley.

and each inverse effective mass component is


1 1 ∂2E
= i, j = x, y, z . (12.69)
m∗ij 2 ∂ki ∂kj

From Eq. (12.66), the energies in the indirect conduction band valleys are differentiated according to
Eq. (12.69) to find, in the case of cubic crystals, that the inverse effective mass tensor reduces to
⎛ ∗ −1 ⎞
mxx 0 0
1
=⎝ 0 m∗yy −1 0 ⎠, (12.70)
m∗ ∗ −1
0 0 mzz

in which the tensor components m∗ij −1 are non-zero only when i = j. The conduction mechanism in a
semiconductor solid is affected by the total effective mass of the carriers, and can be defined by the relation

I = σ •E (12.71)

or by
E = ρ•I, (12.72)
where I is the current vector, E is the electric field vector, σ is the conductivity tensor and ρ is the resistivity
tensor. The unit tensor is simply ⎛ ⎞
1 0 0
σ •ρ = ⎝ 0 1 0 ⎠ , (12.73)
0 0 1
from which it is seen that σ −1 = ρ. The total conductivity is described by

σ= σk (12.74)
Sec. 12.5. Charge Transport 451

and
⎛ ⎞
m∗xx −1 m∗xy −1 m∗xz −1
σ k = (nk q 2 τ ∗ ) ⎝ m∗yx −1 m∗yy −1 m∗yz −1 ⎠ , (12.75)
m∗zx −1 m∗zy −1 m∗zz −1

where nk is the number of free electrons in the equivalent ellipsoids in k-space, σ k is the conductivity
component for ellipsoids in k-space of direction k, q is the unit electronic charge and τ ∗ is the free carrier
mean free drift time. For cubic crystals, the total effective mass always adds up to be the same, regardless
of the direction of force applied to the semiconductor. For instance, a block of semiconducting material
may have parallel electrodes placed at opposite ends of the block. Regardless of the planes upon which the
electrodes are placed, or rather the direction by which an electric field force is applied across the crystal
by an external voltage, the summed effective mass, and consequently the conductivity and charge carrier
mobility, always sum to the same average value for cubic lattice semiconductors. Take for example an indirect
band-gap semiconductor with the lowest conduction band minima in the [100] direction, or at X. The free
carriers are confined in constant energy ellipsoidal surfaces as depicted in Fig. 12.32.
Suppose an electric field force is applied in the [010]
direction, as shown in Fig. 12.34. The common conven- [001]
tion has the electric field vector pointing in the negative kz
direction. As a result, electrons in the ellipsoid surfaces
are pushed towards the [010] direction, as depicted in
Fig. 12.34. The curvature of the energy bands with re- -
spect to k are different in the transverse directions than E [100]
in the longitudinal directions, hence the effective masses
- ky
are also different. By invoking symmetry arguments, [010] [010]
it can be seen from Fig. 12.34 that the force vector is
directed longitudinally along two ellipsoids and trans-
versely along four ellipsoids. The magnitudes of each [100] kx
effective mass tensor component is denoted as m∗l for
longitudinal contributions and m∗t for transverse contri-
butions.
For the conductivity component along the [100] di- -
rection, and by symmetry for the [100] direction, [001]
⎛ ⎞ Figure 12.34. Constant energy ellipsoids for the X valley,
m∗l −1 0 0 depicting the effect of an electric field vector applied in the
[100] 2 ∗ ⎝ ⎠.
σ [100] = σ [100] = (n q τ ) 0 m∗t −1 0 [010] direction. The small dots are for illustration purposes
0 0 m∗t −1 only, depicting that electrons are distributed preferentially
according to the electric field vector.
(12.76)
Similarly, for the remaining axial directions,
⎛ ⎞
m∗t −1 0 0
[010] 2 ∗ ⎝ ⎠
σ [010] = σ [010] = (n q τ ) 0 m∗l −1 0 (12.77)
0 0 m∗t −1

and
⎛ ⎞
m∗t −1 0 0
[001] 2 ∗ ⎝ ⎠.
σ [001] = σ [001] = (n q τ ) 0 m∗t −1 0 (12.78)
0 0 m∗l −1
452 Review of Solid State Physics Chap. 12

All six of the 100 ellipsoids are equivalent energy minima, so that the total number of available con-
duction electrons can be represented by
n0
= n[100] = n[100] = n[010] = n[010] = n[001] = n[001]
6
From Eq. (12.74), each conductivity direction tensor is added to find the summed conductivity tensor, which
yields ⎛ 1: 2 ; ⎞
3 m∗ + m1∗ 0 0
 ⎜
t l : 2 ; ⎟
σ k = (n0 q 2 τ ∗ ) ⎝
1
σ= 0 3 m∗ + m1∗ 0 ⎠, (12.79)
t l
1
: 2 1
;
0 0 3 m∗ + m∗ t l

which can be rewritten as


* +* +⎛ ⎞ * +
1 0 0
n0 q 2 τ ∗ 2 1 ⎝0 1 ⎠ n0 q 2 τ ∗
σ= ∗ + ∗ 0 = 1, (12.80)
3 mt ml m∗c
0 0 1

where 1 is the unit tensor and the conductivity effective mass is defined as the scalar value
* +* +
1 1 2 1
= + ∗ . (12.81)
m∗c 3 m∗t ml
Despite the direction chosen for adding the effective mass tensor components, the result of Eqs. (12.80) and
(12.81) for X valley semiconductors are always the same. Hence, regardless of the direction by which an
electric field is applied to a cubic lattice semiconductor, the conductivity effective mass, m∗c , is always the
same, implying that mobility and conductivity can be treated as constant values for cubic semiconductors.
A similar analysis for L valley semiconductors again produces a constant value for the effective mass, as does
the trivial analysis needed for Γ valley semiconductors.

Example 12.2:
The constant energy ellipsoids of L valley cubic semiconductors, such as Ge, are shown in Fig. 12.31.
Notice, however, they are aligned along the 111 directions. Determine the conductivity tensor for the [111]
direction ellipsoid.

Solution:
A new coordinate system is applied in which one ellipsoid is aligned along a major axis, z  for instance.
In such a case, the new coordinate system can be rewritten in terms of the conventional Cartesian coordinate
system. Each ellipsoid can then be rewritten in its appropriate coordinate representation.
To simplify matters a bit, note that there are eight ellipsoids in Fig. 12.31, but each ellipsoid terminates
in the middle at the Brillouin zone boundary. Therefore, there are only four complete ellipsoids, which can
be redrawn as shown in Fig. 12.35. Taking the ellipsoid labeled A, the z  direction is aligned along the
longitudinal axis, which, using the diagram of Fig. 12.35, the unit vector can be written as
1
iz = √ (ix + iy + iz ). (12.82)
3
The unit vectors for the x and y  directions must be perpendicular to the z  direction and to each other.
The plane they must lie in is depicted in Fig. 12.36. Notice that this plane must also intersect three planes,
namely the zy, the xy, and the xz planes. Any of these intersections can be chosen for the second unit
vector. For the present example, the ky kz -plane is chosen. Vectors in the ky kz plane have no kx component.
Sec. 12.5. Charge Transport 453

kz
kz
[111]
[111]
-
[111]

, ,
kx
ky ,
B A kz
[010] [010]
A
C D ky
ky

kx kx
Figure 12.35. For the effective mass calculation, the Figure 12.36. Coordinate systems used for the example,
eight half ellipsoids for the L valley can be rearranged as showing the relationship between kx , ky and kz to kx , ky
four complete ellipsoids as shown. and kz .

The dot product of the unit vector in this new vector and Eq. (12.82) must vanish, and is a suitable choice
for iy .
Hence, the y  unit vector is
1
iy = √ (−iy + iz ).
2
The x direction unit vector is found from the cross product of iy and iz ,

2 1 1 1
ix = iy × iz = − √ ix + √ iy + √ iz = √ (−2ix + iy + iz ).
6 6 6 6

The unit vectors are arranged in matrix form to redefine the x, y and z unit vectors for the [111] ellipsoid
A, ⎛ 2 ⎞⎛ ⎞ ⎛ ⎞
− √6 √1 1

6 6 ix ix
⎜ 0 1 ⎟⎝ ⎠ ⎝
⎝ − √1
2

2 ⎠
i y = iy ⎠
√1 √1 1
√ iz iz
3 3 3

So the system of equations to determine the original Cartesian coordinates is represented by,
⎛ 2 ⎞⎛ ⎞ ⎛ ⎞
− √6 √1
0 3 ix ix
⎜ √1 1 ⎟⎝  ⎠
⎝ 6 − √1
2

3 ⎠
iy = ⎝ iy ⎠ .
√1 √1 √1 iz iz
6 2 3

A method is now available to describe both coordinate systems in terms of the other. Consider an arbitrary
vector k to be described in both coordinate systems, then
   
k= kj ij , j = x, y, z = km im , m = x, y, z.
j m
454 Review of Solid State Physics Chap. 12

Hence,
   
2 1 1 1 1
k = kx − √ ix + √ iz √ ix − √ iy + √ iz
+ ky
6 3 6 2 3
 
1 1 1
+kz √ ix + √ iy + √ iz .
6 2 3
Now k can be written in terms of kx , ky , kz by collecting the terms from the respective unit vectors,

2 1 1
kx = − √ kx + √ ky + √ kz
6 6 6

1 1
ky = − √ ky + √ kz
2 2

1 1 1
kz = √ kx + √ ky + √ kz
3 3 3
The constant energy surface of ellipsoid A is described by Eq. (12.66)
 2 2


2 (kz − k0 )
 2
kx + ky
E − EC =  + .
2m∗l 2m∗t

Upon setting k0 to 0, and substitution of the terms for kx , ky , and kz one obtains
2 : 2 ;
E − EC = kx + ky2 + kz2 + 2kx ky + 2kx kz + 2ky kz
6m∗l

2 : 2 ;
+ ∗
kx + ky2 + kz2 − 2kx ky − 2kx kz − 2ky kz
3mt
The conductivity tensor for the [111] direction ellipsoid from Eq. (12.69) is,
⎛ ⎞
1 2
  3 m∗
+ m1∗ − 31 m2∗ − m1∗ − 13 2
m∗
− 1
m∗
2 ∗ ⎜ t l t l t l ⎟
n0 q τ ⎜ 1 2 ⎟
σ[111] = ⎜ − 3 m∗ − m1∗ 1
3 m∗
2
+ m1∗ − 13 2
m∗
− 1
m∗ ⎟
4 ⎝ t l t l t l ⎠
− 13 m2∗ − m1∗ − 31 m2∗ − m1∗ 1
3
2
m∗
+ 1
m∗
t l t l t l

The remaining three ellipsoid conductivity tensors must now be calculated and summed together with this
one to find the total conductivity tensor for the L valley. When performed, which is left as a problem exercise,
the result is identical to the result for X valley semiconductors, demonstrating that the conductivity, and
consequently mobility, in a cubic semiconductor is the same regardless of the direction of electrical force.

It should be noted that the result in the above example is not necessarily true for other semiconductor
crystal systems and lattices. Non-cubic semiconductors, such as HgI2 and PbI2 , can have quite different
conductivities and charge carrier mobilities for different k-space directions.
Next the density-of-states effective mass is developed and should not be confused with the conductivity
effective mass. Centering the indirect energy surface ellipsoids at zero, the relation between effective mass
and energy is
2 2 2
E − EC = (k 2
+ k 2
) + k . (12.83)
2m∗t 1 2
2m∗l 3
Sec. 12.5. Charge Transport 455

where the subscripts 1, 2 and 3 can be interchanged for the x, y and z axes. Substitution of

2m∗l 2m∗t
1/2 1/2
a1 = (E − EC ) and a2 = (E − EC )
2 2

into Eq. (12.83), where 2a1 is the length of the major ellipsoid axis and 2a2 is the length of the minor ellipsoid
axis, and division by (E − EC ) yields

k12 + k22 k2
1= + 3.
a2 a1
The “volume” of the ellipsoid in k-space is
4
V = πa1 a22 .
3
Define m∗e as the isotropic effective mass, which is an average effective mass within all of k-space, along with
a spherical constant energy surface bounded by k as shown in Fig. 12.37. The volume of this sphere is
4 3
V = πk ,
3 ef f
where
2m∗e (E − EC )
1/2
kef f = .
2
Equating the ellipsoid volumes in k-space to the isotropic effective mass volume yields
4 4 3
NBZ πa1 a22 = πkef f
3 3

4 2m∗l 2m∗t 4 2m∗e (E − EC )


1/2 3/2
NBZ π (E − EC ) (E − EC ) = π
3 2 2 3 2

NBZ (m∗l m∗t 2 )1/2 = m∗e 3/2 ,

where NBZ is the number of constant energy ellipsoid surfaces lying within the first Brillouin zone. As a
result, the isotropic effective mass for a cubic semiconductor is

m∗e = NBZ (m∗l m∗t 2 )1/3 .


2/3
(12.84)

For the case of Si, there are six ellipsoid surfaces within the first BZ with NBZ = 6, whereas for Ge only
half of each ellipsoid within the first BZ (see Fig. 12.38), resulting in NBZ = 4.
Their effective masses can be described by,

m∗e (Si) = 62/3 (m∗l m∗t 2 )1/3 and m∗e (Ge) = 42/3 (m∗l m∗t 2 )1/3 .

For direct band-gap semiconductors there is only one spherical constant energy surface, and m∗t = m∗l , hence,

m∗e (GaAs) = (m∗l m∗t 2 )1/3 = m∗e ,


456 Review of Solid State Physics Chap. 12

kz
kz
1/8 sphere surface
-
[111]

ky
keff

[010]

ky

kx kx
Figure 12.37. A sphere of constant energy in Figure 12.38. Constant energy ellipsoids for the L valley, depicting
k-space with radius of kef f is used to define m∗e . that only half of each ellipsoid lies within the first Brillouin zone.

where m∗e is the radial effective mass in all directions, because m∗l and m∗t are essentially the same. Overall,
a method of defining an isotropic effective mass is developed, which is commonly referred to as the density-
of-states effective mass.
Next, the effective mass for the holes is addressed. Notice again in Fig. 12.28 that there are three valence
band maxima, of which only two are considered to play an important part in hole conduction. Assuming that
the upper portion of the heavy hole and light hole bands are parabolic and have spherical energy surfaces,
it is usual to write an equivalent effective mass as

m∗h 3/2 = m∗lh 3/2 + m∗hh 3/2 (12.85)

or
m∗h = (m∗lh 3/2 + m∗hh 3/2 )2/3 . (12.86)

Equation (12.86) is only an approximation, because (1) the bands are not actually parabolic at zone center,
nor are the energy surfaces perfectly spherical, and (2) the split-off band may in fact contribute holes to the
conduction process.

12.5.1 Charge Carrier Mobility


The motion of a charge carrier can be influenced by diffusion, scattering, trapping, magnetic fields and
electric fields. The strength of this influence is characterized by the carrier mobility, described as [Sze 1981]
q τci
μi = , i = n or p, (12.87)
m∗i
Sec. 12.5. Charge Transport 457

where τc is the average time between scattering collisions and m∗ is the effective mass of the hole or electron.5
Note that mobility increases with decreasing effective mass. The valence and conduction bands have different
periodic potentials, and for this reason electron mobility in the conduction band is different than hole mobility
in the valence band. Electron mobility is denoted μe and hole mobility is denoted μh .
The speed of a charge carrier can be approximated with
vi = μi E, (12.88)

where E is the electric field magnitude. Equation (12.88) is a good approximation provided that the electric
field is below the saturation field strength (typically below about 2 × 103 V cm−1 ). Above the saturation
field the charge carrier velocities begin to asymptotically approach a limiting or saturation speed. Carrier
velocities for indirect band-gap semiconductors are often described by the empirical formula [Sze 1981],
 γ −1/γ
Eo
v  vs 1 + , (12.89)
E
where vs is the saturation speed and Eo is an experimentally determined constant. Although Eq. (12.89)
may be useful for some semiconductors, such as Si and Ge, it is altogether incorrect for semiconductors
such as GaAs and InP in which more than one band gap may play an important function in the free
carrier population. What is important to understand is that speeds for electrons and holes saturate, usually
somewhere between 6 × 106 cm s−1 and 2 × 107 cm s−1 , depending on the type of semiconductor and dopant
concentration. Consequently, the usefulness of Eq. (12.88) is limited.

12.5.2 Material Resistivity and Capacity


The ability of a semiconductor to conduct electrons is referred to as the material resistivity, with units of
ohm centimeter. The resistivity of a semiconductor is
1
ρ= , (12.90)
q(μe n + μh p)
where q is the unit electronic charge, n and p and the free electron and hole densities, respectively, and μe
and μh are the electron and hole mobilities, respectively. If n p, then Eq. (12.90) reduces to
1
ρ , (12.91)
qμe n
and if p n, then Eq. (12.90) reduces to
1
ρ. (12.92)
qμh p
The resistance of a right parallelepiped block of the semiconductor is
d
R=ρ , (12.93)
A
where d is the detector width or length, and A is the contact area. The parallel plate capacitance for a bar
of semiconductor is found by
o κA
C= , (12.94)
d
5 Often in the literature the subscripts n and p, used to indicate negative and positive charge carriers, are replaced by e and h
to refer, equivalently, to electrons and holes.
458 Review of Solid State Physics Chap. 12

where o is the permittivity of free space and κ is the semiconductor dielectric constant. The RC time
constant of the material, commonly referred to as the dielectric relaxation time, is
ρd o κA
RC = = ρo κ. (12.95)
A d
This is the time needed by a semiconductor to return to electrical neutrality after injection or extraction of
charge carriers.

12.5.3 Intrinsic Semiconductors


Semiconductors that are mostly void of impurities and defects that can alter the electrical characteristics of
the pure material are referred to as intrinsic semiconductors. The term does not necessarily mean a perfect
semiconductor, because materials are intrinsic if the intrinsic properties dominate over extrinsic properties.
The conductivity in an intrinsic semiconductor is dominated by free charge carriers excited directly across
the band gap rather than carriers excited from energy sites appearing in the band gap from crystal defects.
Because the electrons excited into the conduction band come from the valence band, there must be an
equal density of empty states in the valence band. To determine the conductivity of the semiconductor, the
density of filled states in the conduction band and the density of empty states in the valence band must be
determined.
Density of Energy States
To determine the density of energy states, revisit the problem of an electron trapped in a potential well,
discussed in Section 12.3.4, but now with a slight change. The electron is now trapped in a three-dimensional
potential box. The potential box is bounded in the x, y, and z directions by dimensions a, b and c. The
three-dimensional Schrödinger wave equation that describes the possible states of the particle is [Nussbaum
1962],
2 2
− ∇ ψ(x, y, z) + U (x, y, z)ψ(x, y, z) = Eψ(x, y, z), (12.96)
2me
with 0 < x < a, 0 < y < b, and 0 < z < c.
The particle is trapped within the box, from which infinite energy is required to escape, i.e., the particle
has zero potential energy so that U (x, y, z) = 0 within the box. With this simplification, Eq. (12.96) can be
rewritten as
∇2 ψ(x, y, z) + k 2 ψ(x, y, z) = 0, (12.97)
where  <
2me E 2 k 2
k= and E= . (12.98)
 2 2me
To solve Eq. (12.97) employ the method of separation of variables, in which the three-dimensional wave
function is expressed as
ψ(x, y, z) = X(x)Y (y)Z(z). (12.99)
Substitute for ψ in Eq. (12.97) and divide by XY Z to obtain
1 d2 X(x) 1 d2 Y (y) 1 d2 Z(z)
2
+ 2
+ + k 2 = 0. (12.100)
X(x) dx Y (y) dy Z(z) dz 2
For Eq. (12.100) to be valid for a point (x, y, z) in the box, each of the first three terms must equal a constant,
i.e.,
1 d2 X(x)
= −kx2 , 0 < x < a, (12.101)
X(x) dx2
Sec. 12.5. Charge Transport 459

1 d2 Y (y)
= −ky2 , 0 < y < b, (12.102)
Y (y) dy 2
1 d2 Z(z)
= −kz2 , 0 < z < c, (12.103)
Z(z) dz 2
in which
k 2 = kx2 + ky2 + kz2 . (12.104)
The solution of Eq. (12.101), Eq. (12.102), and Eq. (12.103) is subject to the boundary conditions that
X(x), Y (y), and Z(z) must vanish on the surfaces of the potential box. For example, because X(0) =
X(a) = 0 the only solutions of Eq. (12.101) are X(x) = A sin(kx x), where kx = nx π/a, nx = ±1, ±2 ± 3, . . ..
Similar results are obtained for Y (y) and Z(z). In this manner, the solution of Eq. (12.97) is
ψ(x, y, z) = A sin(kx x) sin(ky y) sin(kz z) (12.105)
with
nx π ny π nz π
kx = , ky = , and kz = . (12.106)
a b c
where nx , ny , and nz are integers ±1, ±2, ±3, . . . .
From this solution one can calculate the number of allowed electronic states, per unit volume defined by
the dimensions a, b and c. Recall in reciprocal lattice space, the reciprocal-space unit-cell volume is defined
by
π π π π3
cell volume = = (12.107)
a b c abc
and represents one state or solution. Hence, the number
of solutions per reciprocal space volume is kz
no. of solutions 1 state abc
= 3 = 3. (12.108)
unit cell volume π /abc π k +Dk
Note that the number of solutions per reciprocal space ky
volume does not equal the number of allowed states. k
From Eq. (12.98) and Eq. (12.101) the energy of an al-
lowed state depends on (n2x , n2y , n2z ) so the 8 possible solu-
tions ψ±nx ,±ny ,±nz (x, y, z) all have the same energy level.
Hence, for each unit volume of reciprocal space, the num-
ber of solutions must be divided by the 8 possible combi-
nations of (±nx , ±ny , ±nz ) to get the density of allowed
states. However, because the particles can have 2 values of kx
spin, the allowed states must then be multiplied by 2. As c
b
a result, the density of allowed states within a reciprocal a
space unit volume becomes
Figure 12.39. The number of allowed states can be
no. of allowed states abc modeled as quantum well boxes inside a spherical shell
= . (12.109) in k-space.
unit cell volume 4π 3
To determine the density of allowed states per unit volume in real space, consider a spherical shell in reciprocal
space, as shown in Fig. 12.39, in which the axes are defined by kx , ky and kz . For any particular value of
k = (kx2 + ky2 + kz2 )1/2 , the volume in dk about k is

volume = 4πk 2 dk. (12.110)


460 Review of Solid State Physics Chap. 12

Thus, the number of allowed states within this volume can be estimated as
 
: 2
; abc (abc)k 2 dk
no. of allowed states = 4πk dk = . (12.111)
4π 3 π2
From Eqs. (12.98), 
1 me dE 2 kdk
dk = √ , where dE = . (12.112)
 2 E me
Substitution of these results into Eq. (12.111) gives the density of allowed states N (E)dE with energies
between E and E + dE, namely
√ 3/2
abc 2me √
N (E)dE = 2 EdE. (12.113)
π 3
The density of states N (E), per unit volume and per unit energy
about E, is then obtained by dividing the number of states
N (E)dE by the unit volume per state in dE about E, i.e.,
√ 3/2 √
abc 2me √
3/2
1 2Eme
N (E) = 2 EdE = , (12.114)
π 3 V dE π 2 3
where V = abc.
Finally, because there are no allowed states permitted in
the band gap, substitution of the effective masses for electrons
and holes in Eq. (12.114), yields densities of allowed states for
the conduction and valence bands, namely

2(E − EC )m∗e 3/2
NC (E) = , E ≥ EC , (12.115)
π 2 3
and

Figure 12.40. The density of states for the con- 2(EV − E)m∗h 3/2
duction and valence bands. In the band gap, NV (E) = , E ≤ EV , (12.116)
there are no states, hence NC (E) = NV (E) = 0. π 2 3
where NC (E) is the density of states in the conduction band and NV (E) is the density of states in the
valence band. Here m∗e and m∗h are the effective mass of an electron or hole, respectively. The variation of
these densities with E − EC and EV − E is shown in Fig. 12.40.
Charge Carrier Concentration
Because electrons are fermions, they must obey the Pauli exclusion principle so each state at energy E can
contain at most 1 electron with a given spin. Further, the probability an electron has energy E is governed
by Fermi-Dirac statistics and states that the number n(E) of electrons in quantum states in unit energy
about E per unit volume is given by
n(E) = g(E)fF D (E), (12.117)
where the degeneracy parameter g(E) is the number of states in unit energy about E per unit volume
available to an assembly of electrons and fF D (E) is the Fermi function, named after its discoverer,
1
fF D (E) = . (12.118)
E − EF
1 + exp
kT
Sec. 12.5. Charge Transport 461

Here k is Boltzmann’s constant, T is the absolute temperature, and EF is the Fermi energy. The Fermi
energy is defined as the energy level, at 0 K temperature, for which all states below it are filled and all above
it are empty. Equation (12.118) can be used to determine the density of electrons in the conduction band,
i.e., for E ≥ EC . From Eq. (12.118), it is seen that the probability an electron crosses the band gap to the
conduction band increases with increasing temperature. The Fermi-Dirac distribution is shown in Fig. 12.41.
The free electron density n in the conduction band is
that of the negatively charged carriers, and the free hole den-
sity p in the valence band is that of the positively charged
carriers. The empty states in the valence band are treated
as positive charge carriers called “holes”, a concept which
greatly simplifies calculations. For a pure material, the den-
sity of electrons in the conduction band must equal the
density of holes in the valence band, i.e., n = p. Such a
situation is referred to as the intrinsic case.
The free electron density can be found by integrating the
product of the conduction band density of states function
and the Fermi-Dirac distribution function, namely
 Etop
n= NC (E)fF D (E)dE, (12.119)
EC

where Etop is the top of the first conduction band. Almost


all charge carriers in the conduction band are located near
the bottom of the band with none of the states at the top
filled; hence integration from EC to Etop is equivalent to Figure 12.41. The Fermi-Dirac probability distribu-
tion function. At 0 K, the distribution indicates that
integration from EC to ∞. all energy states above the Fermi energy are empty and
Substitution of Eq. (12.115) and Eq. (12.118) into all states below the Fermi energy level are filled. As the
Eq. (12.119), with the upper integration limit replaced by temperature is increased, the probability of states being
filled above the Fermi energy increases.
∞, gives √ ∗ 3/2  ∞ √
2me E − EC
n= dE. (12.120)
π 2 2 EC 1 + exp[(E − EF )/(kT )]
To evaluate this integral,
√ let ξ = (E − EC )/(kT ), define ηc ≡ (EF − EC )/(kT ), recall that  = h/(2π), and
recall Γ(1 + 12 ) = π/2 [Pierret 1989]. Eq. (12.120) then reduces to
 ∞
2πm∗e kT
3/2
1 ξ 1/2
n=2 dξ,
h2 Γ(1 + 1/2) 0 1 + exp[ξ − ηc ]

2
= NC √ F1/2 (ηc ) = NC F1/2 (ηc ). (12.121)
π
Here NC ≡ 2[2πm∗e kT ]/h2 ]3/2 is energy-independent and referred to as the effective density of states in the
conduction band. The quantity F1/2 is the Fermi-Dirac integral of 1/2 order, while F1/2 is the Fermi-Dirac
integral function of order 1/2.6

6 This particular integral is one of the more important integrals encountered in semiconductor physics and belongs to a general
set of Fermi-Dirac integral functions defined by [Blakemore 1985]
 ∞
1 ξj
Fj (t) = dξ.
Γ(1 + j) 0 1 + exp[ξ − t]
462 Review of Solid State Physics Chap. 12

The density of empty states in the valence band must equal the density of filled states in the conduction
band. Because fF D (E)dE is proportional to the probability of filled states with energy in dE about E
in the conduction band, then the probability of empty states in dE about E in the valence band must be
proportional to [1 − fF D (E)]dE. Because the empty states are near the top of the valence band, the density
p of empty states (or holes) in the valence band is
 EV
p= NV (E)[1 − fF D (E)] dE, (12.122)
Ebot

in which the integral is taken from the bottom of the valence band Ebot to the valence band edge at EV .
Because the empty states are near the top of the valence band with no unfilled states at the band bottom,
the lower limit of integration may be replaced by −∞. Substitution of Eq. (12.116) and Eq. (12.118) into
Eq. (12.122), with the lower integration limit replaced by −∞, gives
√  √
m∗p 3/2 2 EV EV − E
p= dE
π 2 3
−∞ 1 + exp[(E − EF )/(kT )]

2πm∗h kT
3/2
2
=2 √ F1/2 (ηv ) = NV F1/2 (ηv ), (12.123)
h2 π
where ηv = (EV − EF )(kT ). The energy independent term NV is the effective density of states in the
valence band. It is important to note that the use of the Fermi-Dirac distribution function and the results
of Eq. (12.121) and Eq. (12.123) are valid for all positions of the Fermi energy level, EF .
Unfortunately, there are no closed-form analytical expressions for any Fermi function of positive order.
Hence, closed form expressions for Eq. (12.121) and Eq. (12.123) are not available. Numerical integration
may be used to evaluate F1/2 (η) or some approximate expression is used. There are several approximations
for the Fermi-Dirac integral, some far more complex than others. One relatively simple approximation for
the Fermi-Dirac integral of order j = 1/2 is [Pierret 1989]
F1/2 (η)  exp(η) − 0.3 exp(2η) + 0.06 exp(3η) (12.124)
with less than ±0.75% error for negative values of η and less than ±1.5% error for positive values of η no
greater than 0.5.
The results of Eqs. (12.121) and (12.123) are quite general and apply to any semiconductor, doped or
undoped, under the restriction that any added dopants or impurities do not appreciably change the band
structure of the original semiconductor, i.e., the density of states functions of Eqs.(12.115) and (12.116) are
not changed.
Approximations for the Charge Carrier Concentrations
A useful approximation for the non-degenerate case, in which the Fermi energy level is within the band gap
and at least 3kT away from either the conduction or valence band edges, is to approximate the Fermi-Dirac
distribution function fF D (E) by the Boltzmann distribution fB (E), i.e., if E ≥ EC and EC − EF ≥ 3kT
1 EF − E
fF D (E) ≡  exp ≡ fB (E). (12.125)
E − EF kT
1 + exp
kT
With this approximation and Eq. (12.115), the concentration of free charge carriers (electrons) in the con-
duction band is found to be
 ∞  ∞ ∗ 3/2 √ 
me 2 EF − E
n= NC (E)fB (E) dE = 2 3
E − EC exp dE
EC EC π kT
Sec. 12.5. Charge Transport 463

 3/2
2πm∗e kT EF − EC
=2 exp ,
h2 kT

which yields the following useful relation

EF − EC
n = NC exp . (12.126)
kT

In a similar manner the concentration of free charge carriers (holes) in the valence band can be found
approximately with Boltzmann’s approximation. Here an approximation is needed for 1 − fF D (E) when
E ≤ EV and EF − EV > 3kT . In this case

1 E − EF
1 − fF D (E) =  exp . (12.127)
EF − E kT
1 + exp
kT

With this approximation and Eq. (12.116) the concentration p of holes in the valence band is
  √
EV EV
m∗h 3/2 2  E − EF
p= NV (E)[1 − fF D (E)] dE  EV − E exp dE
−∞ −∞ π 2 3 kT
 3/2
2πm∗h kT EV − EF
=2 exp ,
h2 kT

from which the following useful relation is obtained

EV − EF
p = NV exp . (12.128)
kT

Comparison of Eq. (12.126) to Eq. (12.121) and Eq. (12.128) to Eq. (12.123), shows that

F1/2 (η)  eη (12.129)

provided EC − EF ≥ 3kT (or ηc ≤ −3) and EF − EV ≥ 3kT (or ηv ≤ 3).


WARNING: Eq. (12.126) and Eq. (12.128) are only approximations and should not be used for degenerate
semiconductors!7 If the material is intrinsic, i.e., the background impurities have negligible effect upon the
semiconductor properties, then the following must be true for the free carrier concentrations,

Ei − EC EV − Ei
ni = n = p = NC exp = NV exp , (12.130)
kT kT

7A degenerate semiconductor is a heavily doped semiconductor whose Fermi level may no longer be in the energy band gap.
464 Review of Solid State Physics Chap. 12

where ni is the intrinsic free carrier concentration and Ei is the E


intrinsic Fermi energy level.8 From this result it is apparent that

EC
np = n2i . (12.131)
(a) Ei
Equation (12.131) is the so-called mass-action law, and, because EV
it was derived with the Boltzmann approximation, it is only valid fFD(E)
for non-degenerate semiconductors. Equation (12.131) can be used
to derive the intrinsic free carrier concentration of a semiconductor,

EF − EC EV − EF E
n2i = np = NC exp NV exp
kT kT
NC(E)
EV − EC −Eg
= NC NV exp = NC NV exp . EC
kT kT
(b) Ei
where Eg is the band-gap energy. Thus the intrinsic carrier concen-
tration is EV
NV(E)
√ −Eg
ni = NC NV exp . (12.132)
2kT

Notice that the free charge carrier concentration increases exponen- E distribution of
tially with absolute temperature. Notice also that the band gap of a filled states in
semiconductor largely affects the free carrier concentration, in which the conduction band
large band-gap materials has higher electrical resistivity than small E C
band-gap materials, a property that is important for semiconductor (c)
Ei
radiation detectors.
In Fig. 12.42 the Fermi-Dirac function is shown along with the EV
density of states functions, NC (E) and NV (E), and the distribu- distribution of
tion of charge carriers in the conduction and valence bands. No- filled states in
tice in Fig. 12.42(a), that the Fermi-Dirac distribution is symmetric the valence band
about the Fermi energy level, i.e., there are just as many filled states
Figure 12.42. Shown are (a) the Fermi-
above EF as there are empty states below√EF . Notice also that the Dirac function for an intrinsic semiconduc-
density of states function increases with E from the band edges, tor, (b) the density of states functions, and
as required by Eqs. (12.115) and (12.116), and that there are no (c) the distribution of free charge carriers,
states in the band gap. As a result, the product, fF D (E)NC (E), electrons and holes, in the conduction and
valence bands, respectively.
or [1 − fF D (E)]NV (E) is zero in the band gap. Further, as NC (E)
or NV (E) increases with E, the probability of a state being filled
decreases with increasing E. Hence, the product fF D (E)NC (E) is non-linear, as is the distribution of free
charge carriers in the conduction band and the valence band, as shown in Fig. 12.42(c).
The total number of free carriers excited from the valence band to the conduction band per unit time in a
semiconductor crystal depends upon the band gap energy, temperature, and the actual volume of the crystal.

8 The intrinsic Fermi level Ei is a constant for a given semiconductor and equals the actual Fermi level EF if impurities are
negligible. However, as impurities or dopants are added the Fermi level changes although the intrinsic Fermi level remains
constant.
Sec. 12.5. Charge Transport 465

Hence, one can quickly surmise that, given a limit on allowable leakage current, wide band-gap materials
have lower leakage currents from thermal generation of charge carriers than narrow band-gap materials.
Further, under ideal conditions, wide band-gap materials can be fashioned into larger devices than narrow
band-gap materials, and they can still exhibit low leakage currents. Lastly, for narrow band-gap materials,
the operating temperature of the material can be reduced so as to lower the leakage current, as is usually
done with Ge and large Si devices.

12.5.4 Impurities and Extrinsic Semiconductors


One of the more useful properties of semiconductors is that their electrical conductivities can be altered with
the simple addition of various impurities. Depending on the valence of the impurity atoms and the host
semiconductor, the electrical conductivity can be dominated by hole motion or electron motion. Further, with
proper concentrations, impurities can be added to an unintentionally contaminated (doped) semiconductor
to make it behave much like an intrinsic semiconductor.

electrons
EC EC EC
ED
EF p-type
EF n-type dopant states
dopant states (filled)
(empty) EF
EA
EV EV EV
intrinsic holes n-type p-type
Figure 12.43. The simplified energy band structures for intrinsic, n-type, and p-type
materials. The electron and hole carrier concentrations are equal for the intrinsic case.
Materials doped n-type have an excess of electrons in the conduction band, and materials
doped p-type have an excess of holes in the valence band.

Dopant Impurities
Dopant impurities are often added to a semiconductor to control its electrical properties. Dopants that
add excess electrons to the chemical binding are called donors, because they need only a slight amount of
thermal energy to transfer these excess electrons into the conduction band. Dopants that lack an electron
to complete the valence bonding are called acceptors, because they need only a slight amount of energy
to accept electrons from the valence band into their unfilled states. The simplified energy band structures
for intrinsic, n-type, and p-type materials are depicted in Fig. 12.43. The concentration of donor atoms
is denoted by ND with energy level ED , and the concentration of acceptor atoms is denoted by NA with
energy level EA . If donors are added to the semiconductor, then the concentration of holes is reduced. The
opposite occurs if acceptors are added to the semiconductor. Because dopants are generally used in such a
small concentration that the energy band structure is unaffected, the general relationship between the free
electron concentration and the free hole concentration is given by Eq. (12.131).
Background
In the preparation and the growing of crystals, there are many ways contaminant atoms can enter the crystal
even after rigorous purification processes. Typically, a variety of processes are used to remove contaminants
from the starting crystal material. These include vapor distillation, zone melting, and zone refinement. All
466 Review of Solid State Physics Chap. 12

of these methods depend upon an ability to diffuse impurity ions from one region of the starting material to
another. Often the segregation coefficients of impurities is not conducive to such processes and the impurities
are, therefore, hard to remove. Ge and Si can be purified to levels below one ppb with zone refinement and
float zone refinement. However, inadequate handling techniques can reintroduce impurities from chemicals
used for growth preparations, crucibles and ampoules used during the growth process, heating coils and
liners in the growth furnaces, as well as human introduced impurities such as Na and K. These undesirable
impurities are commonly referred to as background impurities.
Although the presence of impurities generally affects the electronic performance of a semiconductor
material, the effect can vary widely. For instance, some impurities may introduce scattering centers that
can affect the free carrier mobility, but may not be electrically active, i.e., they do not introduce free charge
carriers to the conduction or valence bands. For example, boron impurities in GaAs, in high concentrations,
can affect the mobility of the charge carriers, but they are electrically inactive. As a result, pyrolitic BN is
often used as the crucible for GaAs bulk crystal growth. By contrast carbon, sources of which are present in
practically all steps of the GaAs materials preparation and crystal growth, is an electrically active shallow
acceptor and behaves as a p-type dopant. Hence, carbon affects mobility and electrical conductivity.
If the background impurities, primarily those that are electrically active, can be kept to levels below
the intrinsic free carrier concentration of the semiconductor of interest, then the material still behaves in-
trinsically. However, extrinsic behavior is observed for impurity concentrations approaching or exceeding
the intrinsic concentration. Often impurities of opposite electrical behavior are purposely added during the
crystal growth process to counteract the effect of background impurities, a process referred to as compen-
sation. Dopants may also be added during post-growth processes, such as implantation and diffusion, so as
to intentionally dope a semiconductor to behave as n-type or p-type. Under such processes, select regions
of a semiconductor sample may be doped n-type while other regions of the same sample are doped p-type.
Selective doping allows for the formation of rectifying and ohmic junctions.
Extrinsic semiconductors are those materials whose electrical properties are dominated by impurity atoms
and intrinsic defects. Typically, there is a temperature range in which extrinsic semiconductors demonstrate
such behavior, beyond which the thermal excitation of charge carriers directly from the valence band causes
the material to behave intrinsically. At the top of Fig. 12.44 are depictions of the free carrier concentrations
for intrinsic material (ni ), lightly doped material (n or p), and highly doped material (n+ or p+ ). At low
temperatures, the shallow donor and acceptor sites are not fully ionized, a region referred to as the freeze-out
region.
As shown in the bottom of Fig. 12.44, as the temperature is increased, more of the impurities become
ionized, until they are all ionized. In the extrinsic region, few electrons are excited from the valence band to
the conduction band, hence the extrinsic carrier concentration from impurities far exceeds the free carrier
concentration excited from the valence band. At this point the material behaves extrinsically, i.e., the
conductivity remains largely unchanged and is dominated by the concentration of impurities present in the
semiconductor. An important aspect to impurity doping is that it allows the device designer to control the
semiconductor electrical conductivity over a wide temperature range, something that cannot be done with
intrinsic materials in which the free carrier concentration changes exponentially with temperature.
As the temperature is increased further, thermal generation increases the density of free carriers excited
from the valence band to the conduction band until they surpass the free carrier density excited from impurity
sites, and the material behaves intrinsically. The temperature at which the crossover from extrinsic to
intrinsic behavior is located increases as the impurity concentration increases. Hence, highly doped materials
retain extrinsic behavior at higher temperatures than do lightly doped materials.
Sec. 12.5. Charge Transport 467

EC EC EC EC
many all

few few many


EV EV EV EV

freeze out transition extrinsic intrinsic

Figure 12.44. At low temperature, the impurities do not have enough thermal energy to become
fully ionized, a temperature region known as freeze-out. As the temperature is increased, there is
a transition in which the shallow impurities become ionized. At a high enough temperature, the
thermal energy fully ionizes the shallow impurities, although the thermal energy is not enough to
promote significant electron excitation from the valence to conduction bands. As a result, in the
extrinsic region, the conductivity of the semiconductor is controlled, and limited, by the impurity
concentration. At higher temperatures, the concentration of electrons excited from the valence
band exceeds the impurity concentration, and the conductivity is controlled by the intrinsic free
carrier concentration.

Degeneracy Factors
In the earlier use of the Fermi-Dirac distribution it was assumed that each available state could be occupied
by only one electron. However, an electron occupying states in the band gap, whether donor or acceptor
sites, can have either spin-up or spin-down, so that there are two different methods by which the state might
be filled. As a result, the donor state is said to have a degeneracy gD of 2. Typically, only one conduction
band plays a dominant role in charge conduction, hence the Fermi-Dirac function is corrected for degeneracy,
468 Review of Solid State Physics Chap. 12

and the ionized donor concentration is


ND ND
+
ND = ND [1 − fF D (ED )] = ND − = . (12.133)
1 ED − EF EF − ED
1+ exp 1 + 2 exp
gD kT kT

Recall that there are two active valence bands in cubic semiconductors; hence, there is a degeneracy of 2
for the spin states multiplied by a degeneracy of 2 for the overlapping heavy hole and light hole bands from
which the electrons can fill the acceptor states. Typically, the hole degeneracy of a band-gap state, gA , is
assumed to be 4, thereby yielding

NA NA
NA− = NA fF D (E) = = . (12.134)
EA − EF EA − EF
1 + gA exp 1 + 4 exp
kT kT

With these results one can now determine free carrier concentrations and conductivities for shallow dopant
impurities.
Degeneracy values for deep levels in a band gap are far more difficult to determine, because impurity
atoms can give rise to numerous energy states in a band gap. Typically, for deep donors, deep acceptors and
traps, the ionized concentrations are written as

NDD − NAA NT
+
NDD = , NAA = and NT∗ = .
EF − EDD EAA − EF EF − ET
1 + gDD exp 1 + gAA exp 1 + gT exp
kT kT kT

where the subscripts DD and AA are used for deep donors and deep acceptors, respectively, and the subscript
T is used for charge carrier traps. Depending on the lattice site into which an impurity atom falls, the
impurity may act as a donor or an acceptor, complicating matters more. It is usual for a degeneracy of 1 to
be assigned to deep donors, deep acceptors and traps; however, one should be aware that such an assumption
could be seriously incorrect.
Shallow Dopant and Shallow Impurity Energy Levels
Atoms in a semiconductor crystal that are purposely introduced are commonly referred to as dopant atoms;
whereas, those impurities that are inadvertently present as a consequence of the starting material or growth
and handling processes are usually referred to as background impurities. In either case, the impurities
can alter the electrical behavior of the host semiconductor, whether it is through changes in electrical
conductivity, charge carrier mobility, or charge carrier mean free drift times. Ge, Si, and GaAs energy
levels have been studied extensively, and energy levels associated with impurities and defects are shown in
Tables 12.3, 12.4, and 12.5. Numerous other semiconductors used for radiation detectors have also been
studied, yet the energy levels and associated impurities and defects are still under investigation.
A block of semiconductor material, whether it is intrinsic, n-type or p-type, must have the same number
of negative and positive charges, because the material must have zero overall charge. This charge neutrality
arises because any free electron with negative charge has an original host atom that became a positive ion,
and for every free hole, there is an acceptor atom that became a negative ion. Additionally, every negative
electron excited from the valence band to the conduction band leaves behind a positive hole in the valence
band. This charge neutrality condition can be written, with the use of Poisson’s equation, as
ρ q  
∇E = = p − n + ND
+
− NA− = 0, (12.135)
κo κo
Sec. 12.5. Charge Transport 469

Table 12.3. Energy levels (eV) reported as donors and acceptors for Ge (Eg =
0.66 eV). Donors are referenced from the conduction band edge (EC − ED ) and
acceptors are referenced from the valence band edge (EA − EV ). Data are from
[Milnes 1973] and [Sze 1981].

ID n-type p-type ID n-type p-type

Al 0.01 In 0.011
Ag 0.13, 0.38, 0.57 Li 0.0093
As 0.013 Mn 0.16, 0.37
Au 0.62 0.15, 0.46, 0.62 Ni 0.23, 0.36
B 0.01 O 0.04, 0.2
Be 0.02, 0.06 P 0.012
Cd 0.055, 0.16 Pt 0.04, 0.2, 0.54
Cr 0.07, 0.12 S 0.18
Cu 0.04, 0.33, 0.4 Se 0.14, 0.28
Co 0.36, 0.57 0.25 Sb 0.0096
Fe 0.31, 0.39 Te 0.11, 0.3
Ga 0.011 Tl 0.01
Hg 0.087, 0.23 Zn 0.035, 0.095

Table 12.4. Energy levels (eV) reported as donors and acceptors for Si (Eg = 1.12
eV). Donors are referenced from the conduction band edge (EC − ED ) and acceptors
are referenced from the valence band edge (EA − EV ). Data from [Milnes 1973] and
[Sze 1981].

ID n-type p-type ID n-type p-type

Ag 0.79 0.76 Mn 0.43, 0.59 0.45


Al 0.067 Mo 0.33, 0.78, 0.82
As 0.054 Na 0.77
Au 0.83 0.58 Ni 0.23, 0.77
B 0.045 O 0.16, 0.51 0.41, 0.74
Ba 0.32 0.5 P 0.045
Be 0.17, 0.42, Pd 0.34
0.87, 1.01 Pb 0.17 0.37
Bi 0.069 Pt 0.82 0.36, 0.87
C 0.25 S 0.26 0.48
Cd 0.45 0.55 Se 0.25, 0.4
Co 0.35, 0.49, 0.59 Sb 0.039
Cr 0.41 Si 0.63, 0.93 0.78
Cs 0.3 0.5 Sn 0.25 0.27
Cu 0.24, 0.4, 0.53 Sr 0.28, 0.62
Fe 0.14, 0.51. 0.72 Ta 0.14, 0.43
Ga 0.072 Te 0.14
Ge 0.27, 0.62 Ti 0.21
Hg 0.79, 0.87 0.76, 0.81 Tl 0.26
In 0.16 V 0.49 0.4
K 0.26, 0.77 W 0.22, 0.3, 0.37,
Li 0.033 0.78, 0.81
Mg 0.11, 0.25 Zn 0.26, 0.57
470 Review of Solid State Physics Chap. 12

Table 12.5. Energies levels (eV) reported as donors and acceptors for GaAs (Eg = 1.42
eV). Donors are referenced from the conduction band edge (EC − ED ) and acceptors are
referenced from the valence band edge (EA − EV ). Data are from [Milnes 1973], [Sze 1981],
and [Pantelides 1992].

ID n-type p-type ID n-type p-type

Ag 0.11 Mg 0.028
AsGa (EL2)∗ 0.75, 1.0 Mn 0.095
Au 0.09 Ni 0.21
Be 0.028 O 0.4, 0.75∗∗
C 0.026 Pb 0.12
Cd 0.035 S 0.006
Co 0.16 Se 0.006
Cr 0.79 Si 0.006 0.03, 0.1, 0.22
Cu 0.023, 0.14, 0.19, Sn 0.006 0.17
0.24, 0.44 Te 0.03
Fe 0.37, 0.52 V 0.22
Ge 0.006 0.04, 0.07 Zn 0.031
Li 0.023, 0.05
∗ EL2 means “energy level 2”, associated with an intrinsic anti-site defect AsGa .
∗∗ Has at times been confused with the EL2 level.

+
where n is the free electron concentration, p is the free hole concentration, ND is the ionized donor concentra-

tion and NA is the ionized acceptor concentration. Substitution of Eq. (12.126), Eq. (12.128), Eq. (12.133),
and Eq. (12.134) into Eq. (12.135) yields

EV − EF EF − EC ND NA
NV exp − NC exp + − = 0. (12.136)
kT kT EF − ED EA − EF
1 + 2 exp 1 + 4 exp
kT kT

For any specified temperature T , the concentrations, ND +


, NA− , NC , and NV can be calculated. With
these values p and n can be found as shown below. Finally, numerical iteration of Eq. (12.126) can be used
to determine an exact value for the Fermi energy level EF .
For the situation in which donors are the majority impurities, so that ND NA , then with the use of
Eq. (12.126),

ND N ND
n  ND
+
= =   D = n , (12.137)
EF − ED n EC − ED 1+
1 + gD exp 1 + gD exp Nξd
kT NC kT

where  
NC (EC − ED )
Nξd = exp − . (12.138)
gD kT
Equating the first and last terms of Eq. (12.137) and with some algebraic rearrangement, one obtains

n2 + nNξd − Nξd ND = 0, (12.139)


Sec. 12.5. Charge Transport 471

whose solution for positive n is


 1/2  1/2 
2
Nξd Nξd Nξd 4ND
n=− + + Nξd ND = 1+ −1 . (12.140)
2 4 2 Nξd

In a similar fashion, it can be shown that when NA ND ,


 1/2   
Nξa 4NA NV (EA − EV )
p= 1+ −1 , with Nξa = exp − . (12.141)
2 Nξa gA kT

Example 12.3: Suppose Si is doped with shallow donors at a concentration of ND = 1016 cm−3 . It is
known that the donor site is 0.04 eV below the conduction band energy EC . What is the electron free carrier
concentration at 77 K and at 300 K?

Solution:
From Eq. (12.84) and the effective mass m∗l and m∗t values in Table 16.4 for Si at 4 K, the density of states
effective mass at 77 K is estimated to be,
m∗e  62/3 (m∗l m∗2
t )
1/3
= 62/3 ((0.9163)(0.1905)2 )1/3 = 1.062me
where me is the mass of a free electron. Then from Eq. (12.120)
3/2  3/2
2πm∗e kT 2π(1.062me k)(77 K)
NC = 2 = 2 = 3.57×1018 cm3 .
h2 h2
Substitution into Eq. (12.141) gives
3.57×1018 cm3 −0.04 eV
Nξd = exp = 4.3×1015 cm3 .
2 (77 K)(8.617 × 10−5 eV K−1 )
Finally, substitution of these values into Eq. (12.140) gives the free carrier concentration
 1/2 
4.3 × 1015 4(1016 cm−3 )
n(77 K) = 1+ − 1 = 4.75 × 1015 cm3 .
2 4.3 × 1015 cm3

From this result it is seen, at the cryogenic temperature of 77 K, 47.5% of the shallow donor atoms
are ionized; hence, the material is still conductive and behaving extrinsically. If one wishes to design a
detector with low free-carrier densities, as is needed for large-volume low-leakage current devices, it is often
not enough to simply cryogenically cool the material; the semiconductor must also be purified so that only
low concentrations of background impurities are present.
With the same calculations as above, the following results are obtained for T = 300 K: m∗e = 1.084me ,
NC = 2.83 × 1019 cm−3 , Nξd = 3 × 1018 cm−3 , and n(300 K) = 9.97 × 1015 cm−3 . These values indicate
that, at room temperature, almost all (99.7%) of the shallow donor states are ionized. Hence, at room
+
temperature ND  ND .

The result in the above example can be used to simplify calculations for the free carrier concentrations.
In the case that one dopant impurity concentration far exceeds the other type, it can be assumed that, at
room temperature,
n  ND if ND NA or p  NA if NA ND . (12.142)
472 Review of Solid State Physics Chap. 12

For shallow dopants and impurities, the donor and acceptor states are almost completely ionized at room
temperature. The free electron and hole concentrations, n and p, can be obtained from the condition of
charge neutrality, i.e.,
p − n + ND+
− NA− = 0. (12.143)
Then from the mass-action law of Eq. (12.131), p = n2i /n, and Eq. (12.143) can be rewritten as

n2 − n(ND
+
− NA− ) − n2i = 0. (12.144)

This quadratic equation for n is readily solved for n > 0 as


   2 1/2
+
ND − NA− +
ND − NA−
n= + + n2i . (12.145)
2 2

In a similar fashion, the hole concentration is found to be


   2 1/2
NA− − ND
+
NA− − ND
+
p= + + n2i . (12.146)
2 2

+
In the extrinsic region, where ND ni then Eq. (12.145) reduces to
+
ND − NA−
n=2  ND
+
 ND when ND NA . (12.147)
2

Similarly, where NA− ni , Eq. (12.146) reduces to

NA− − ND
+
p=2  NA−  NA when NA ND . (12.148)
2

In the intrinsic region, where ni +


ND or ni NA− , then Eq. (12.145) and Eq. (12.146) reduce to

n  ni and p  ni . (12.149)

From the previous analysis, one can also determine the location of the Fermi level EF . If ND = 0 and
NA = 0 then n = p = ni and EF = Ei . Then from Eqs. (12.126) and (12.128)

EF − EC EV − EF
NC exp = NV exp . (12.150)
kT kT
Upon setting EF = Ei and taking the logarithm of both side of this equation, one obtains
 
NC EV + EC − 2Ei
ln = , (12.151)
NV kT

from which the intrinsic Fermi level is found to be


   
EV + EC kT NV
Ei = + ln . (12.152)
2 2 NC
Sec. 12.5. Charge Transport 473

E E
donor
states
EC EC
(a) EF
(a)
EF
EV EV
fFD(E) fFD(E)
acceptor
states

E E
NC(E) NC(E)
EC EC
(b) (b) EF
EF
EV EV
NV(E) NV(E)

E distribution of E distribution of
filled states in filled states in
the conduction band the conduction band
EC EC
EF
(c) (c)
EF
EV EV
distribution of distribution of
filled states in filled states in
the valence band the valence band

(1) (2)
Figure 12.45. Shown are (a) the Fermi-Dirac distributions for extrinsic semiconductors,
(b) the density of states functions, and (c) the distribution of free charge carriers, electrons
and holes, in the conduction and valence bands, respectively. The distributions in column
(1) are for p-type material and the distributions in column (2) are for n-type material.

From Eqs.(12.121) and (12.123), it is seen that NV /NC = (m∗h /m∗e )3/2 so that
 
EV + EC 3kT m∗h
Ei = + ln . (12.153)
2 4 m∗e
In the freeze-out region, one can equate Eq. (12.126) and Eq. (12.140) and solve for EF to obtain
$  1/2 /
Nξd 4ND
EF = EC + kT ln 1+ −1 . (12.154)
2NC Nξd

Similarly, from Eqs. (12.128) and (12.141), one finds


$  1/2 /
Nξa 4NA
EF = EV − kT ln 1+ −1 . (12.155)
2NV Nξa
474 Review of Solid State Physics Chap. 12

Finally, in the extrinsic region one must first relate the intrinsic Fermi level Ei to the actual Fermi level.
From Eq. (12.130) one has NC = ni exp[(EC − Ei )/kT ]. Substitution of this result into Eq. (12.126) gives

EF − Ei
n = ni exp . (12.156)
kT

Similarly from Eq. (12.130), it is seen that NV = ni exp[(Ei − EV )/kT ]. Substitution into Eq. (12.128) then
gives
Ei − EF
p = ni exp . (12.157)
kT
The solution of these two equations for EF in terms of n or p is

EF = Ei + kT ln(n/ni ) = Ei − kT ln(p/ni ). (12.158)

For the case ND NA and ND ni , Eq. (12.158) reduces to

EF = Ei + kT ln(ND /ni ), (12.159)

and for the case NA ND and NA ni

EF = Ei − kT ln(NA /ni ). (12.160)

The Fermi levels and charge carrier distributions for p-type and n-type materials are depicted in Fig. 12.45.
Deep Dopant, Impurity and Defect Energy Levels
Impurities and dopant atoms, as well as intrinsic defects such as antisites, vacancies, and interstitials, can
introduce energy levels deep in the band gap of a semiconductor. Deep donors, acceptors, and traps are
usually characterized as having an energy level greater than 0.1 eV from either band edge within the band
gap. Unlike shallow energy levels, deep levels should not be assumed to be fully ionized at room temperature,
and the Fermi-Dirac distribution function must be used to determine the fraction of deep states that are
filled or empty.
Suppose a semiconductor exists in which there is only one deep level distributed throughout a material
with a concentration of NDD and a shallow acceptor level, NA , of minimal concentration. The electron
concentration is given by
NC EF − EC
n=  NC exp , (12.161)
EC − EF kT
1 + exp
kT
and the density of neutral deep donor sites is

0 NDD
NDD = , (12.162)
1 ED − EF
1+ exp
gDD kT
0
where NDD is the filled or neutral deep donor concentration. With the assumption that the shallow levels
are fully ionized, and because the semiconductor total charge density must be neutral, the following balance
relation holds
NDD − NDD0
− NA − n + p = 0. (12.163)
Sec. 12.5. Charge Transport 475

The density of ionized deep donors is


⎡ ⎤
⎢ 1 ⎥ NDD
+
NDD = n + NA − p = NDD − NDD
0
= NDD ⎢
⎣1 −
⎥=
⎦ .
1 ED − EF EF − ED
1+ exp 1 + gDD exp
gDD kT kT
(12.164)
To find the free electron concentration n, first consider the quantity R ≡ nNDD
+
/(NDD − NDD
+
). Because
the hole concentration is negligibly small, Eq. (12.163) gives
+
nNDD n(n + NA )
R= = . (12.165)
NDD − NDD DD − n − NA
+
N
From Eq. (12.161) and Eq. (12.164) one also finds
+
nNDD NC EDD − EC
R= = exp . (12.166)
NDD − NDD
+
gDD kT
Equating these two expressions for R leads to a quadratic equation in n whose solution for positive n can
be written as
  " 2
gDD NA EC − EDD gDD NA EC − EDD
n = 2(NDD − NA ) × 1+ exp + 1+ exp
NC kT NC kT

#1/2 −1
4gDD (NDD − NA ) EC − EDD
+ exp (12.167)
NC kT
Equation (12.167) can be simplified further by assuming NA to be negligibly small such that NA  0,
  1/2 −1
4gDD NDD EC − EDD
n  2NDD 1 + 1 + exp . (12.168)
NC kT
Equation (12.168) provides a simple expression for the expected free electron concentration in the presence
of a dominating deep donor level.
The opposite case is true if a deep acceptor is present with concentration NAA and with a negligible
number of shallow levels, either for ND and NA . Use of the same arguments used above to find n gives the
hole concentration under the constraint that NAA ND , namely,
  " 2
gAA ND EAA − EV gAA ND EAA − EV
p = 2(NAA − ND ) 1 + exp + 1+ exp
NV kT NV kT
#1/2 −1
4gAA(NAA − ND ) EAA − EV
+ exp (12.169)
NV kT
Equation (12.169) can be simplified if it is assumed that NA is negligibly small so that NA  0,
  1/2 −1
4gA NAA EAA − EV
p  2NAA 1 + 1 + exp . (12.170)
NV kT
Notice that the deep donor and acceptor impurities may not be completely ionized at room temperature (300
K); hence, the actual ionized concentrations must be calculated when determining the free carrier densities
and material resistivities.
476 Review of Solid State Physics Chap. 12

Deep Level Compensation


In the case of wide band-gap semiconductors, the free carrier concentration is typically low for the intrinsic
material. Almost all wide band-gap semiconductors are compound materials with the exception of diamond
which has a band gap of 5 eV. As a result, purification of wide band-gap semiconductors can be complicated.
For example, Si and Ge are widely used semiconductors for radiation detectors. Both are materials composed
of a single element and both can be prepared from a melt process in which a single crystal is grown by changing
it directly from the liquid to solid state. Hence, both Ge and Si can be purified and processed as a single
element. Zone refined Ge and Si has the impure regions removed after purification processes, remelted and
grown into single crystals.
However, the case is not so simple for CdTe, which is a far more complex compound semiconductor. Both
starting materials, Cd and Te, are typically purified separately. Afterwards, the purified materials must be
reacted to form the compound CdTe, which unfortunately is never quite complete because there is always
a small percentage of free Cd and free Te left in the molten material. The situation is further complicated
by noting that segregation coefficients for some impurities in Cd may be negligible in Te. Hence, when the
two are mixed, an impurity efficiently removed from one (Cd, for instance) may be introduced by the other
element (Te in this example). Further, during growth, a Cd atom may fall into a Te location or vice versa,
thus forming antisites that behave as electrically active impurities, a condition that does not occur for Si or
Ge.
It is also important to be able to control the electrical properties of semiconductors that are to be used
for radiation detectors. After purification, if the background doping levels remain too high, often impurities
are added that act as deep impurities. Deep impurities have energy levels that fall deep in the band gap of
a semiconductor, typically greater than 0.1 eV from the band edge. Often the most effective deep dopants
have energy levels near the middle of the band gap.
Two-Level Model: In the case of two levels present in the semiconductor, for instance one shallow acceptor
level and one deep donor level, a simplified compensation model can be developed for the free electron density
in the conduction band [Lindquist and Ford 1982],
 
1 (EA − EC )
n NC exp , (12.171)
x−1 kT

where x = NA /NDD .
Three-Level Model: Suppose one wants to compensate a material that has been unintentionally doped
with p-type dopants from background contamination. In addition, suppose there is a residual concentration
of n-type dopants as well, such that NA > ND . It is desired to add the correct amount of deep level donors
to the semiconductor with the goal of making the material have a high resistivity. Hence, the goal is to force
the Fermi energy level to the middle of the band gap, as shown in Fig. 12.46. For this example, the three
level model is used in which NDD > NA > ND [Blanc and Weisberg 1960; Lindquist and Ford 1982]. Charge
neutrality and Eq. (12.131) require

n2i
+
n = p + ND +
+ NDD − NA− = +
+ ND +
+ NDD − NA− . (12.172)
n
+
At room temperature ND  ND and NA−  NA . Hence, with the use of Eq. (12.162),
Sec. 12.5. Charge Transport 477

n2i NDD n2i


n = NDD (1 − f (EC − EDD )) − (NA − ND ) + = − (NA − ND ) + . (12.173)
n EF − EDD n
1 + gDD exp
kT

If it is assumed that n ni , the last term in the above re-


sult can be neglected. Then substitution of Eq. (12.126) into EC
Eq. (12.173), with the last term set to zero, gives ED
EC − EDD EF
NC NDD exp − EDD
kT
(NA − ND ) + n = . (12.174)
EC − EDD EA
ngDD + NC exp − EV
kT

If the condition exists such that NA − ND n, then Figure 12.46. The basic three-level compensa-
tion model with two shallow levels and one deep
level. Depicted is the case in which NDD > NA >
EC − EDD
NC NDD exp − ND , in which the deep levels are only partially
kT ionized. In such a case, the Fermi energy level
(NA − ND )  . (12.175)
EC − EDD is “pinned” near the middle of the band gap,
ngDD + NC exp − thereby producing a relatively higher resistivity
kT material.

The solution of this equation for ngDD gives

EC − EDD
NC (NDD − 1) exp −
kT
ngDD  . (12.176)
(NA − ND )

Finally, if NDD 1, then the above result reduces to

EC − EDD
NC NDD exp −
kT
n , (12.177)
gDD (NA − ND )

which gives an approximation for the expected free electron concentration in the conduction band for deep
donor compensated material.
Using a similar argument, compensation with deep acceptor levels is achieved if NAA > ND > NA .
Through a similar, but opposite, system of equations, the resulting concentration of free holes is,

EAA − EV
NV NAA exp −
kT
p . (12.178)
gAA (ND − NA )

Example 12.4:
The semiconductor GaAs is a moderately wide band-gap material (eV = 1.42 eV) that has been used
for radiation detector development. Bulk grown material even in its purest form often has background
impurities. Typically, GaAs is compensated by purposely incorporating excess As in the melt to give rise
to the intrinsic anti-site defect, AsGa , which produces a deep donor level in the material 0.75 eV below the
478 Review of Solid State Physics Chap. 12

conduction band edge (denoted EL2). Carbon, a shallow acceptor, appears as a background contaminant in
concentrations near 1015 cm−3 , with shallow n-type materials appearing in concentration near 1014 cm−3 .
What is the room temperature free electron concentration if the EL2 concentration is 1016 cm−3 ?

Solution:
Substitution of given values into Eq. (12.177) with gDD = 2 yields

0.75 eV
(4.7 × 1017 cm−3 )(1016 cm−3 ) exp −
(300 K)(8.617 × 10−5 eV K−1 )
n = 9.482 × 104 cm−3 .
2(1015 cm−3 − 1014 cm−3 )

With μe  8000 cm2 V−1 s−1 , this free electron concentration thus results in a resistivity from Eq. (12.91)
of approximately ρ = 8.24 × 109 ohm cm.

12.6 Summary
Solid state materials used for radiation detectors are generally composed of crystalline materials. A crystalline
material is defined by a basis of atoms arranged upon a periodic lattice. There are 14 possible Bravais lattice
systems. The periodic arrangement of atoms causes the appearance of periodic potentials. This potential
periodicity causes bands of allowed states to form, producing quasi-continua of energy states in these bands.
The density of allowed energy states in these bands is defined by the density of states function. Gaps between
these bands are referred to as energy gaps. The energy band that plays the part of atomic bonding is the
valence band, and the energy band that plays the part in electron conduction is the conduction band. The
energy gap between the valence band and the conduction band is referred to as the band gap.
Energy bands have maxima and minima when defined by energy and crystal momentum in what are
known E-k diagrams. Empty states in the valence band are treated as positive particles called “holes”. Be-
cause electrons need only lose energy to recombine with a hole in direct band gap semiconductors, the charge
carriers have high recombination probabilities, thereby causing short charge carrier lifetimes. Electrons must
change both momentum and energy to recombine with holes for semiconductors with indirect band gaps;
hence, the charge carrier lifetimes are generally longer than observed for direct band-gap materials. Bands
with sharp curvature d2 E/dk 2 cause the charge carrier effective mass for electrons or holes to decrease.
Small effective mass increases the charge carrier mobility. The electrical behavior of semiconductors can be
controlled by introducing dopant impurities. Deep dopants can be added into material to increase resistivity
and reduce leakage currents in such a way that the material performs in a similar fashion as intrinsic material.
The introduction of excess impurities or defect centers causes a reduction in charge carrier lifetime.

PROBLEMS

1. For the structure shown in Fig. 12.47, what are the Miller indices for the listed planes?
(a) BSFT, (b) HMNP, (c) OTHO, (d) JVCW, (e) OKGR, (f) LTEL, (g) KSFO, (h) HTBP, (i) OTSO,
(j) LFEL, (k) OKHP, (l) HFSP

2. For the structure shown in Fig. 12.47, what are the direction indices for the following directions?
(a) OT, (b) LV, (c) SJ, (d) NK, (e) OJ, (f) LF, (g) SM, (h) NT
Problems 479

H G F
J M
V
K
T
E
A D
L
P R
W S
c a N C
b B

Figure 12.47. Lattice structure.

V(x)

I II III IV
V(x)
V0

I II III
V=0 V0
a

-V0

-a x=0 -a 0 a

Figure 12.48. Potential well Figure 12.49. Potential well.


and barrier.

3. For a cubic unit cell, find the angles between the normals to the pairs of planes defined by the following
Miller indices

(a) (100)(010), (b) (100)(111), (c) (100)(210), (d) (110)(210)

4. For the cubic lattice systems, determine the reciprocal lattice vectors a∗ , b∗ and c∗ for the FCC lattice
and the BCC lattice.

5. For the potential shown in Fig. 12.48, solve for the reflection and transmission coefficients.

6. Quantum well cavities can be formed by growing consecutive layers of varying semiconductors that have
different band-gap energies. For instance, a quantum well can be defined by epitaxially growing a layer
of AlGaAs, with a band gap of 1.71 eV, followed by GaAs, with a band gap of 1.42 eV, followed by
another AlGaAs layer. Typically, such films are only a few tens to hundreds of angstroms thick, and are
grown on semiconductor buffer layers with protective contacts on top. Fig. 12.49 shows a square well
where a = 50 Å, V0 = 0.3 eV, and m∗ = 0.06 m0 . Find the following: (a) Find the allowed energies of
the states in the well. (b) Find the wave functions and coefficient values. (c) Plot the wave functions for
the allowed energies. (d) Determine the probabilities that an electron is located at the allowed energies.
480 Review of Solid State Physics Chap. 12

7. Show that the solution to the Kronig-Penney model can be reduced to Eq. (3.58). Here is a hint to make
matters simpler: Assume that the barrier is a delta function such that φ k such that d2 u/dx2 du/dx
in the region, and simplify.

8. For a 2-dimensional square lattice, draw the first 4 Brillouin zones and clearly show their boundaries.
Perform the same exercise for a 2-dimensional hexagonal lattice.

9. Determine the conductivity effective mass for cubic lattice L valley semiconductors by completing the
example problem 12.2.

10. A silicon sample is doped with boron at a concentration of 5 × 1015 cm−3 . What is the expected
resistivity of the material at a temperature of 194 K? What is it at a temperature of 300 K?

11. A silicon sample is doped with a concentration of 1016 cm−3 phosphorus atoms. At 300 K, what are
the concentrations of free electrons and holes?

12. InP (Eg = 1.35 eV) is often doped with Fe (EC − EAA = 0.66 eV) to increase resistivity. With
NA = 3 × 1014 cm−3 , ND = 2.5 × 1015 cm−3 , and NAA = 1.5 × 1016 cm−3 , what is the expected
resistivity?

REFERENCES
BLAKEMORE, J.S., Solid State Physics, 2nd Ed., Cambridge: LIMA DE FARIA, J., Ed., Historical Atlas of Crystallography, Dor-
Cambridge University Press, 1985. drecht: Kluwer Academic Publishers, 1990.
BLANC, J. AND L.R. WEISBERG, “Energy Level Model for High- LINDQUIST, P.F. AND W.M. FORD, “Semi-Insulating GaAs Sub-
Resistivity Gallium Arsenide,” Nature, 192, 155–156, (1960). strates,” Ch.1, in GaAs FET Principles and Technology, J. V.
BLOCH, F., “Über die Quantenmechanik der Elektronen in DILORENZO AND D.D. KHANDELWAL, Eds., DedHam: Artech
Kristallgittern,” Z. Physik, 52, 555–600, (1928). House, 1982.

BRAVAIS, A., “Mémoire sur les Systèmes Formés par les Points MCKELVEY, J.P., Solid State and Semiconductor Physics, New
Distribués Rguliérement sur un Plan ou Dans L’espace” J. Ecole York: Academic Press, 1966.
Polytech., 19, 1-128, (1850).
MILLER, W.H., A Treatise on Crystallography, Cambridge: Pitt
BRILLOUIN, L., Wave Propagation in Periodic Structures, 2nd. Press, 1839.
Ed., New York: Dover, 1953.
MILNES, A.G., Deep Impurities in Semiconductors, New York:
DE FARIA, J.L., Ed., Historical Atlas of Crystallography, Dor- Wiley, 1973.
drecht: Kluwer Academic Publishers, 1990.
NUSSBAUM, A., Semiconductor Device Physics, Englewood Cliffs:
GASIOROWICZ, S., Quantum Physics, New York: Wiley, 1974. Prentice Hall, 1962.
KITTEL, C., Introduction to Solid State Physics, 6th Ed., New
York: Wiley, 1986. PANTELIDES, S.T., Deep Centers in Semiconductors, 2nd Ed.,
Philadelphia: Gordon and Breach, 1992.
KITTEL, C., Solid State Physics, A Short Course, New York: Wi-
ley, 1966. PIERRET, R.F., Advanced Semiconductor Fundamentals, Read-
ing: Addison-Wesley, 1989.
KRONIG R. DE L. AND W.G. PENNEY, “Quantum Mechanics of
Electrons in Crystal Lattices,” Proc. R. Soc. Lond. A, 130, SZE, S.M., Physics of Semiconductor Devices, 2nd Ed., New York:
499–513, (1931). Wiley, 1981.
Chapter 13

Scintillation Detectors
and Materials

In a few minutes there was no doubt about it. Rays were coming
from the tube which had a luminescent effect upon the paper.
I tried it successfully at greater and greater distances, even at
two meters. It seemed at first a new kind of invisible light.
It was clearly something new, something unrecorded.
Wilhelm C. Röntgen

13.1 Scintillation Detectors


Because Röntgen used a scintillating platinobarium cyanide plate to discover x rays in 1895, scintillation
radiation detectors hold the distinction of being the first type of radiation detector ever invented. However,
the emission of light was basically a qualitative measure of radiation interactions and not so much a quan-
titative measure. The fluorescence of the material indicated the presence of penetrating ionizing radiation,
yet the actual intensity of radiation was not easily gauged.
Materials that scintillate are generally separated into two classes, namely inorganic and organic. The
method by which either produces scintillation light is physically different, hence the distinction. Inorganic
scintillators can be found as crystalline, polycrystalline, or microcrystalline materials. Organic scintillators
come in many forms, including crystalline materials, plastics, liquids and even gases.
The scintillation principle is quite simple. Radiation interactions in a scintillator cause either the atomic
or molecular structure in the scintillator to become excited such that electrons are increased in potential
energy. These excited electrons then spontaneously de-excite with the decrease in potential energy emitted
as radiant light energy. These light emissions can then be detected with light sensitive instrumentation.
Although simple in concept, there are certain attributes that a material must possess to be a useful
scintillator. First, the material must be capable of absorbing the radiation of interest. Second, the subsequent
energy released from the scintillator must be largely radiative, i.e., a large percentage of the absorbed
energy is converted to photons. Third, the light emission must be spontaneous such that the scintillator
fluoresces rather than phosphoresces.1 Fourth, the scintillator must be transparent to its own scintillation
light. Finally and fifth, the fluorescent light must be of a wavelength that can be detected with conventional

1 Phosphorescence is a process in which light emission continues after the source of radiation is removed

481
482 Scintillation Detectors and Materials Chap. 13

light detecting systems, such as photomultiplier tubes or semiconductor photodiodes. There are many
materials that scintillate, but only a select few have all of the necessary properties listed above. In fact,
many scintillators were discovered and used in a limited sense for the first 50 years after Röntgen’s discovery
of x rays.
Many early discoveries depended on the observation of scintillation light. Wilhelm Röntgen used such
light to discover x rays and Ernest Rutherford counted, through a microscope, flashes of light produced
in a scintillating screen from alpha particle interactions in it.2 Although scintillators were well known to
be sensitive to radiation, their relatively low light yields made them difficult to use as practical detectors.
Further, light detection devices needed to detect the scintillations were inadequate at the time. As a result,
gas filled detectors dominated the detector industry prior to the 1940s.
An attempt to couple special Geiger-Müller counter tubes with scintillators is described by Krebs [1934,
1941] (also see [Daggs et al. 1952]), who used a thin window GM counter as a light detection device. A
screen coated with zinc sulphide (ZnS) was the scintillator used by Krebs, and over the following years many
other scintillators were also investigated by Krebs and other researchers [Mandeville and Scherb 1950, Krebs
1955]. However, GM tubes do not preserve energy deposition information, and these types of scintillation
detectors served only as radiation counters.
In 1941, RCA introduced the first commercial photo-multiplier tube (PMT), a highly light-sensitive
electron-amplification vacuum tube that could detect tiny amounts of visible light. In was the PMT that
enabled scintillating materials to become practical radiation spectrometers. With improvements in stability
and spectral response, eventually it was the PMT that became the light detector of choice for scintillators.
In 1944, Curran and Baker and later Broser and Kallman [1947a, 1947b] and Coltman and Marshall
[1947] successfully used PMTs coupled to scintillators to measure alpha, beta, and gamma radiation. Broser
and Kallman [1947b] and Deutsch [1948] used the organic scintillator naphthalene, because it was trans-
parent to its own light emissions, to measure ionizing radiations.3 In 1948 Robert Hofstadter discovered
NaI:Tl, probably the most important scintillator in use over the last 65 years. The first efficient gamma-ray
scintillation counters and spectrometers were demonstrated when a NaI:Tl crystal and a PMT were coupled
together [Hofstadter 1948, 1949; McIntyre and Hofstadter, 1950; Hofstadter and McIntyre, 1950].
A typical scintillation spectrometer consists of a scintillating material hermetically sealed in an internally
light-reflecting canister. Typical canisters are cylindrical, with an optically transparent window at one end
of the cylinder and all remaining surfaces are Lambertian reflectors.4 The optically transparent window
is coupled to a light collection device, such as a PMT, with an optical compound. The optical compound
helps match the indices of refraction between the scintillation canister and the light collection device so as to
reduce reflective losses. The PMT provides a voltage output that is linear with respect to the light emitted
from the scintillator. Hence, the voltage output “spectrum” is a linear indication of the radiation energy
spectrum deposited in the detector. It is typical for commercial vendors to provide the scintillation canister
and the PMT as one complete unit, although they can be acquired separately. Properties of commonly used
inorganic scintillator materials are listed in Table 13.1.

13.2 Inorganic Scintillators


Inorganic scintillators depend primarily on the crystalline energy band structure of the material for the
scintillation mechanism. In Fig. 13.1 an energy band diagram is shown for a typical inorganic scintillator.

2 This fatiguing process led Hans Geiger and Rutherford to invent the Geiger gas-filled detector.
3 Hofstadter notes in his 1975 review paper that “all nuclear physics laboratories smelled of mothballs” shortly after Broser and
Kallman [1947b] published their work.
4 A Lambertian surface, named after Johann Heinrich Lambert, has luminance independent of the angle of view. Typically

these reflectors are white and not glossy or mirror-like.


Sec. 13.2. Inorganic Scintillators 483

Table 13.1. Widely used inorganic scintillator materials with some of their properties.

Density Refractive λmax Decay Light Yield Bi-Alkali PMT


Scintillator (g/cm3 ) Index (nm) Time (photons Response Reference
(at λmax ) (ns) per MeV) WRT NaI(Tl)
Alkali Metal Halides
CsI - fast 4.51 1.95 315 16 2000 0.04–0.06 S
CsI - slow 4.51 1.95 450 1000 ∼200 ND S
CsI:Na 4.51 1.84 420 460, 630, 41000–49000 0.85 S, D
1800
CsI:Tl 4.51 1.79 550 600, 3500 54000–61000 0.45 S, M
LiI:Eu 4.08 1.96 475 1400 15000 0.35 S2
NaI:Tl 3.67 1.82 415 230 43000 1.00 S
Alkali Earth Halides
BaF2 - fast 4.88 1.54 220 0.6–0.8 1800 0.03 S
BaF2 - slow 4.88 1.5 310 630 10000 0.16 S
CaF2 :Eu 3.18 1.44 435 900 24000 0.50 S
CaI2 3.96 1.8 410 550 86000 ND H
CaI2 :Eu 3.96 1.8 470 790 86000 ND H
CaWO4 6.1 1.94 425 8000 ∼20000 0.3-0.5 Z
SrI2 :Eu 4.55 1.85 435 1200 115000 ND C
Transition Metal Scintillators
CdWO4 7.90 2.30 470 14000 ∼1350 0.3–0.5 S
ZnS:Ag 4.09 2.36 450 110 50000 1.3 S
Post-Transition Metal Scintillators
Bi4 Ge3 O12 7.13 2.15 480 300 8200 0.13 S
Lanathanide Scintillators
CeBr3 5.2 2.09 371 17 68000 ND R
Gd2 SiO5 6.71 1.85 440 56, 400 9000 0.20 L
LaCl3 :Ce 3.86 2.05 350 28 49000 0.70–0.90 S
LaBr3 :Ce 5.29 2.05 380 16 63000 1.65 S
Elpasolites
Cs2 LiYCl6 3.31 1.81 305 6600 6535, 22420 ND C2
Cs2 LiYCl6 :Ce 3.31 1.81 372, 400 600, 6000 9565, 18400 ND C2
Cs2 LiLaBr6 :Ce 4.2 1.85 420 180, 1100 43000 1.15 S
Cs2 LiLa(Br,Cl)6 :Ce 4.08 1.9 420 120, 500, 1500 45000 ∼ 0.70 B2
Garnets, Perovskites, and Orthosilicates
LuAlO3 :Ce 8.34 1.94 365 16.5, 74 11400 ND M
Lu3 Al5 O12 :Pr 6.71 1.84 310 20-22 ∼18000 ND N, D2
Lu2 SiO5 :Ce 7.4 1.82 420 47 25000 0.75 L
Lu1.8 Y.2 SiO5 :Ce 7.1 1.82 420 41 32000 0.75 S
YAlO3 :Ce 5.35 1.95 370 27 18000 0.45 B
Y3 Al5 O12 :Ce 4.55 1.82 550 88, 302 17000 0.50 S
Y2 SiO5 :Ce 4.45 1.8 420 56 24000 ND L
Ceramic Scintillators
Li glass:Ce 2.5 1.55 395 (n) 18, 57 ∼4650 ∼0.12 S1
(α) 16, 49
(β) 20, 58
Tb glass 3.0–3.52 1.5–1.62 550 3 ms–5 ms 13000–50000 P
B: Baryshevsky et al. 1991; B2: BNC 2020; C: Cherepy 2009; C2: Combes 1999; D: de Haas 2005;
D2: Drozdowski 2008b; H: Hofstadter 1964a, 1964b; L: Leroq et al. 2005;
M: Moszynski 1997a, 1997b; N: Nikl 2013; P: Pavan 1991; R: Shah 2005; R2: Shah 2017;
S: Saint-Gobain 2016; S1: Scintacor 2016; S2: Syntfeld 2005; Z: Zdesenko 2005
484 Scintillation Detectors and Materials Chap. 13

Upper
Band

Forbidden
Band

Conduction
Band

Ec
Exciton Band Exciton Band
Et1a
Et1b
Band
Exciton

Exciton
Eg Eg
Gap

Et0
Ev
Valence Band

Forbidden
Band
Tightly Bound
Band

(A) (B)
Figure 13.1. Shown are two basic methods by which an inorganic scintillator produces light,
(A) is the intrinsic case and (B) is the extrinsic case.

A lower energy band, referred to as the valence energy band, has a reservoir of electrons. It is this band
of electrons that participates in the binding of atoms. The next higher band is usually referred to as the
conduction band, which for inorganic scintillators is usually devoid of electrons. Between the two bands is a
forbidden region where electrons are not allowed to exist, typically referred to as the energy band gap.
If a radiation particle, such as a gamma ray or charged particle, interacts in the scintillation material, it
can excite numerous electrons from the valence band and the tightly bound bands up into the conduction
bands as shown in Fig. 13.1(A). These electrons rapidly lose energy and fall to the conduction band edge
EC . As they de-excite and drop back into the valence band, they can lose energy through light emissions.
Unfortunately, because the radiated energy of the photons is equivalent to the band-gap energy, these same
photons can be reabsorbed in the scintillator and again excite electrons into the conduction band. Hence, the
scintillator usually is opaque to its own light emissions. There are exceptions in which intrinsic scintillators
work well. For example, bismuth germanate (BGO) releases light through optical transitions of Bi+3 ions,
which release light that is lower in energy than the band gap, hence is relatively transparent to its own light
emissions.
However, if an impurity or dopant is added to the crystal, it can produce allowed states in the band gap,
as depicted in Fig. 13.1(B). Such a scintillator is referred to as activated. In the best of cases, the impurity
atoms are uniformly distributed throughout the scintillator. When electrons are excited by a radiation
event, they migrate through the crystal and many subsequently drop into the excited state of the impurity
atom. Upon de-excitation, a photon is produced equal in energy to the difference between the impurity
atom’s excited and ground states. Hence, it is unlikely to be reabsorbed by the scintillator material. Careful
Sec. 13.2. Inorganic Scintillators 485

selection of the proper impurity dopant can allow the light emission wavelength to be tailored specifically to
match the sensitivity of the light collection device.

13.2.1 Theory of Scintillation for Inorganic Scintillators


The scintillation process is described elsewhere as consisting of five distinctive stages [Rodyi 1997], namely
1. Radiation absorption and subsequent excitation of electron-hole pairs.
2. Relaxation of primary electron-hole pairs.
3. Thermalization of the low-energy of charge carriers.
4. Energy transfer to luminescent centers.
5. Photon emission from the luminescent centers.
It is difficult to observe the separate processes of stages 1 through 3 and stages 4 and 5. Instead, these
processes are usually categorized as electron-hole production followed by photon emission. But, for the sake
of completeness, all five stages are presented here.
Already presented in Chapter 4 are the basic processes by which radiation interacts in matter, and they
are the same for scintillators. An ionizing particle excites multiple electron-hole pairs (see Chapter 12) by
multiple ionizing processes including photoionization, elastic and inelastic scattering, Coulombic scattering,
fission, and neutron transmutation. If the discussion is restricted to photon interactions, then the probability
of exciting a K-shell electron is generally higher than exciting electrons from outer shells (L or M). The process
by which the holes relax is either from radiative transitions, in which an outer shell electron falls into the
empty state by releasing a photon (a characteristic x ray), or by a non-radiative transition (i.e., Auger
electron emission). These subsequent emissions can be reabsorbed by outer shell electrons of nearby atoms,
thereby producing more electron-hole pairs.
Meanwhile, the liberated energetic electrons travel through the crystal lattice and lose energy through
Coulombic interactions and, thus, liberate more electron-hole pairs. The process continues until the resultant
electrons and holes no longer have sufficient energy to produce more ionization. Overall, electrons and holes
move to their respective band edges, electrons at the conduction band edge and holes at the valence band
edge, within about 10−15 to 10−13 seconds.
Excited electrons still bound to their respective holes through Coulombic forces are also formed at this
stage. This condition causes the electron-hole pair to have slightly lower energy than a free electron-hole
pair. Thus, the pair exists at an energy below the band gap energy and can be represented as a temporary
energy band perturbation traditionally called the exciton band, through which the electron-hole pair diffuse
together as an electrically neutral quasiparticle called an exciton.
The intrinsic case (A) has no added activator dopants. Absorbed radiation energy excites electrons from
the valence and tightly bound bands up into the higher energy conduction bands. These electrons quickly
de-excite to the lowest conduction band edge EC . As they drop to back to the valence band, they release
light photons. Some intrinsic scintillators emit light through optical transitions from ionized elemental
constituents, which can be of lower energy than the band gap. The extrinsic case (B) has activator dopants
that produce energy levels in the band gap. Absorbed radiation energy excites electrons from the valence
and tightly bound bands up into the higher conduction bands. These electrons quickly de-excite to the
lowest conduction band edge EC as in case (A). However, many drop into the upper activator site energy
state Et1 . As they then drop to the activator ground state Et0 , they release light photons of lower energy
than the scintillator band gap.
Emission Spectra
The emission spectrum is largely affected by the band-gap energy of the scintillator and the energy levels
of the activator. Moreover, the emission spectrum is usually spread over a continuous range of energies
486 Scintillation Detectors and Materials Chap. 13

E
excited

Intensity (relative units)


Dl
(Stokes Shift)

ground
D
D’
hwe
excitation emission
E2
B Sehwe
hnin C

E1 hnout
E0
hwg
E lmax1 lmax2
Sghwg
Wavelength
A D Qe0 Q

Figure 13.2. Configuration coordinate diagram for a luminescent center depicting


luminescence with a Stokes shift and also a form of non-radiative de-excitation. The
ordinate is energy E and the abscissa is the average distance Q between the luminescent
center and the surrounding ions.

rather than concentrated at discrete energies. As shown in Fig. 13.2, an electron can be excited from
the lowest energy state of a fluorescent center by a photon, it may capture a free electron, or it may
capture an exciton to produce an excited electron at B. When produced by the absorption of a photon,
this electron excitation is a vertical transition and, according to the Franck-Condon principle, occurs nearly
instantaneously (femtoseconds). Because electrons are significantly less massive than the surrounding nuclei,
the electron transition probabilities can be calculated with the assumption that the nuclear positions appear
stationary during the transition. However, after the transition, thermal motion and the relocation of electron
spatial positions cause vibrational states to appear, represented as horizontal lines in Fig. 13.2.
In inorganic scintillators, the photon assisted transitions are broadened, which, in turn, results in a
widening of the luminescent bands [Rodnyi 1997]. If the luminescent center and its nearest ion neighbor can
be modeled by Hooke’s Law,5 then the total energy of the ground state can be modeled as [Yamamoto 2007],

Q2
Ug = kg (13.1)
2
and the total energy of the excited state is,

(Q − Qe0 )2
Ue = ke + E0 , (13.2)
2
where kg and ke are force constants of the chemical bonds, Qe0 is the interatomic distance when the ground
state is at equilibrium, and E0 is the total energy at Q = Qe0 . At location B, the total energy can be
represented by
(Δ)2
Ue = ke + E0 . (13.3)
2
where Δ = QA − Qe0 = −Qe0 .
Elevation of an electron from the ground state to an excited state moves the electron into a different
orbital. Consequently, spatial occupancy and the electron wavefunction changes with this transition from

5 In classical physics, Hooke’s Law describes the stored energy in a spring as a function of displacement, U = kx2 /2.
Sec. 13.2. Inorganic Scintillators 487

the ground state to the excited state. The electron also affects its neighboring atoms differently in its excited
state, resulting in a change in the chemical binding (and force constant k), and the position of lowest energy
changes from A to Qe0 (shown in Fig. 13.2). Further, the potential energy curve of the excited state is wider,
thereby allowing the ground state to come close or overlap the excited state potential energy curve at point
D → D .
An excited electron moves from point A to point B. This excited electron rapidly loses energy and moves
to location C. It can now drop directly to the ground state at location E, thereby releasing a photon.
The electron then loses energy, by non-radiative processes, to once again fall to location A. Ground state
transitions are possible from the several vibrational energy states in the excited state. Consequently, there
is usually a wide range of energies contributing to the emission spectrum, which appears as a continuous
broad spectrum rather than discrete energy emissions.
The excitation energy (A → B) is larger than the emission energy (C → E). This change causes the
resultant absorption spectrum of a luminescent center to be different than the emission spectrum because the
absorption spectrum is centered about shorter wavelengths than is the centroid of the emission wavelengths.
This shift in wavelength is known as the Stokes shift,

Δλ = λmaxem − λmaxab , (13.4)

where the subscripts em and ab indicate emission or absorption, respectively. If the Stokes shift is adequately
large, photon emissions have too little energy to be reabsorbed by the scintillation crystal or other luminescent
centers.
The vibrational states can be modeled as a harmonic oscillator bound by the energy wells depicted
in Fig. 13.2, in which discrete energy states appear within the energy wells. The solutions give rise to
vibrational energy states separated by the phonon energy ω,6 where ω is the vibrational mode angular
frequency [Rodyni 1997], with even and odd wave functions for both of the wells,

1
Eng,e = (n + )ωg,e , n = 0, 1, 2, . . . , (13.5)
2
where the g and e subscripts indicate either the ground or excited potential wells.
In Fig. 13.2, the case is shown in which the number of vibrational states involved with transition A → B →
C, denoted by Se , is different than the number of vibrational states involved with transition C → E → A,
denoted by Sg . The energy and number of phonons involved with the relaxation from B → C are

(Qe0 − QA )2
Se ωe = ke . (13.6)
2
In a similar fashion,
(QA − Qe0 )2
Sg ωg = kg . (13.7)
2
Note that in Fig. 13.2, QA = 0. Suppose that the vibrational frequencies and force constants are the same for
the ground and excited states, such that kg = ke and ωg = ωe , then Se = Sg and the total energy difference
between the transition A → B and the transition C → E is

ΔE = ω(Sg + Se ) = 2Sω, (13.8)

6 Here  ≡ h/(2π) and is widely used to avoid repeated factors of 2π in quantum calculations.
488 Scintillation Detectors and Materials Chap. 13

where S is the number of phonons involved with the absorption or emission of photons, named the Huang-
Rhys factor S [Huang and Rhys 1950]. The Stokes shift becomes,

4πSωc2
Δλ = . (13.9)
Eo2 − (2ω)2

At a given temperature T , the transition probability for phonon absorption is [Yamamoto 2007],

1 −(ω − E1 )2
Wab (ω) = √ exp 2 , (13.10)
2πσab 2σab

where k is Boltzmann’s constant,

ke Q2e0 (ωe )3
E1 = E0 + , and [σab (T )]2 ≈ 2Se kT . (13.11)
2 (ωg )2

Here the spectral absorption width is defined as the FWHM of the Gaussian distribution, wab = 2.355σab .7
For emission, the terms become [Ridley 1982],

1 −(ω − E3 )2
Wem (ω) = √ exp 2
, (13.12)
2πσem 2σem

where
kg Q2e0 (ωg )3
E3 = E0 − = E0 − Sg ωg and [σem (T )]2 ≈ 2Sg kT . (13.13)
2 (ωe )2
If ωe ≈ ωg , then the variance as a function of temperature is,

[σem (T )]2 ≈ 2Sg kT ω, (13.14)

which defines the spectral broadening of the emission spectrum, wem = 2.355σem . From Eq. (13.14), it is
observed that the variance of the emission spectrum increases with Sg , ω, and the absolute temperature T .
It is important that the choice of scintillator matches well to the choice of light sensing device. Perhaps
the most common device employed to detect the relatively low light emissions from a scintillation is a photo-
multiplier tube, or PMT (covered in the following chapter). In Fig. 13.3, there are numerous emission spectra
from common scintillator materials along with two comparison sensitivity responses for two types of PMTs.
There is at least one characteristic that must be considered when coupling a PMT to a scintillator, mainly,
that the spectra match well. For example, the emission spectrum from thallium doped NaI (or NaI:Tl)
matches well to both the S-11 and the K-bialkali PMT responses. However, neither the responses from the
S-11 or K-bialkali PMT match to the CsI:Tl emission spectrum.
Often the potential energy curves depicted in Fig. 13.2 either intersect or come into close proximity along
the Q direction, represented as points D and D . With thermal agitation, the electron can move to the
ground state without releasing a photon. This process can be understood with the assistance of Fig. 13.2, in
which electrons are excited from the ground state of a luminescent center to an excited state (A → B). The
electron quickly moves to the lowest potential energy of the excited state C. If the excited electron acquires
thermal energy equivalent to E2 , it can be raised to point D and transfer to point D , thereby allowing the

7 The spectral absorption width is defined here as the FWHM of the Gaussian distribution, or 2 2 ln(2)σab . However, the
spectral√width has been defined elsewhere as w where Wab (E1 )/q = Wab (E1 + w). Hence, under this alternative definition,
wab = 2σab [Yamamoto 2007].
Sec. 13.2. Inorganic Scintillators 489

" "
'()* (""
   
0-,+
-./
" +,% !
     

  #$%& 
0+,+

!


 +,

,% 
0/,+


+- 


 
       

    

Figure 13.3. The emission spectra from several popular inorganic scintilla-
tors. Also shown is an overlaying sensitivity comparison to the normalized
responses of two common photomultipliers (K-bialkali and S-11). Scintillation
spectral response data from [Lindow et al. 1978, Shah et al. 2005; Valais et al.
2007, and Saint-Gobain 2016]. PMT response data from [Engstrom 1980].

electron to pass directly from the excited state into the ground state without releasing a photon. The excess
energy is lost to thermal lattice vibrations (phonons). Ultimately, these electrons are lost to the luminescent
process and do not contribute to the fluorescent light yield. The loss of these electrons, acting as information
carriers, and the consequential light reduction is called quenching.
There are other competing processes that reduce the fraction of electrons contributing to the overall
fluorescent scintillation spectrum. Electrons may fall into energy states that produce metastable states,
whose transitions to the ground state are forbidden. With some additional energy, these electrons may
move to higher allowed energy states and, thereby complete the radiative process. For instance, thermal
energy from the ambient environment may be enough to cause these transitions. If these delayed transitions
take a relatively long time, beyond several decay times for fluorescent photons, then the radiant decay is
called phosphorescence or afterglow. Phosphorescence becomes a form of background noise in scintillation
detectors. These afterglow light emissions can be detected, but the time delay for the emission decouples its
correlation to the radiation event that caused the initial electron excitations. Note that some light-emitting
materials use phosphorescent decay for benefit, such as the thermoluminescent detectors (TLDs) discussed
in Chapter 19.

13.2.2 General Properties of Inorganic Scintillators


Price [1964] suggests that the charge measured at the output of the light collection device be represented by,

Q = M qne , (13.15)

where M is the multiplication factor of the light collection device (see Chapter 14), q is the electron charge,
and
ne = En Fn Cnp Tp Fp Sm f Fc , (13.16)
490 Scintillation Detectors and Materials Chap. 13

where En is the energy of the radiation quantum, Fn is the fraction of energy deposited in the scintillation
medium, Cnp is the conversion efficiency of energy to fluorescent light, Tp is the transparency of the scintillator
to its own light emission spectrum, and Fp is the fraction of light photons that reach the light collection
sensor. The terms Sm f Fc pertain to the conversion efficiency of the light sensor, where Sm is the light to
photoelectron conversion, f is a factor that corrects for spectral mismatch of the light output to the light
sensor photoresponse, and Fc the photoelectron collection efficiency. Equation 13.15 can be rewritten as,

Q = q(M Sm f Fc )(En Fn Cnp )(Tp Fp ) = qNe Lp Lc . (13.17)

The term Ne (charge production) is mostly addressed in Chapter 14, whereas the terms Lp (light production)
and Lc (light collection) are addressed in this chapter.
Radiation Absorption Efficiency
The radiation absorption efficiency is a strong function of the atomic number and density of the material
constituents. For gamma-ray detection, the three most important radiation interactions in a scintillator are
photoelectric absorption, Compton scattering, and pair-production. For these three interactions, high Z
values produce more efficient results than low Z values. There are some materials that have one moderately
high Z constituent and one or more low Z constituents. Yet it is still the concentration of high Z elements
that largely determines the absorption coefficient. For instance, the absorption coefficient for CsI (55/53) is
only slightly higher than that for NaI (11/53) by about a factor of two or less.
Photoelectric absorption edges should also be considered when selecting a scintillator material for low
energy gamma-ray detectors. Within some energy regions, a scintillator with a relatively large Z constituent
may actually have lower absorption than another scintillator with lower Z constituents. For instance, the
highest K edge for LSO (lutetium orthosilicate) is located at 63.3 keV below which its absorption coefficient
drops from 66.87 cm−1 to 12.86 cm−1 . By comparison, the highest K edge for NaI is located at 33.16 keV.
Consequently, the gamma-ray absorption efficiency is actually higher for NaI than LSO between 33.16 keV
and 63.3 keV.
The exponential attenuation of uncollided gamma rays entering a scintillating crystal is given by Eq. (4.4),
namely
I(x) = Io e−μt (E)x , (13.18)
where Io is the initial gamma-ray intensity intersecting the material surface and x is the distance into the
crystal material. Recall from Chapter 4 that the total interaction coefficient is given by

μt (E) = μi (E) ≈ μpe + μcs + μpp (13.19)

where the subscripts pe, cs, and pp refer to photoelectric, Compton scattering and pair-production, respec-
tively. Note that other gamma-ray interactions are possible, as described in Chapter 4, but are less important
to general gamma-ray detection. In the detector community, the ratio I(x)/Io is called the interaction effi-
ciency and is the probability a photon interacts in some manner in the material while traveling a distance x
in it.
Note the interaction efficiency describes the probability of an interaction, and not the amount of energy
absorbed. A gamma ray absorbed through the photoelectric effect passes its energy (minus the electron
binding energy) to a photoelectron. As the ionized atom de-excites, bound electrons fall into lower energy
levels giving off x rays. These x rays may be reabsorbed in the medium from electrons in higher energy
levels (L and M shells), or may in fact escape the material altogether. Gamma rays that interact through
Compton scattering do not deposit their total energy. In fact, the fractional amount of energy deposited per
scatter decreases as the gamma-ray energy increases. These concepts are described in detail in Chapter 4 and
Sec. 13.2. Inorganic Scintillators 491

their consequences for radiation detection in Chapter 20. In summary, the absorption efficiency describes
the probability of a photon interaction and not the probability that gamma rays are fully absorbed.
For other radiations, lower Z materials may be of more importance. For instance, the backscatter
probability increases with Z for both α and β particles. Thus for a high Z material these radiations have
a good chance of reflecting off the material rather than entering the detector and being detected. Hence,
scintillators used for charged particle detectors are usually fabricated from low Z materials, such as organic
scintillators. For fast neutrons, low Z materials facilitate higher energy loss per collision. Hence, organic
scintillators, such as plastic scintillators, are usually used for fast neutron detectors. When doped with
reactive materials with high absorption cross sections in the thermal region, these scintillators can be used
for slow neutron detection. There are special scintillators with constituent materials that offer excellent
thermal neutron absorption, such as lithium iodide (LiI) and gadolinium oxysulfide (Gd2 O2 S).8

Light Yield
Light yield is the number of fluorescent photons produced per energy unit absorbed in a scintillating medium.
The absolute light yield is the total number of fluorescent photons released per unit absorbed energy, typically
reported as photons per MeV. The absolute light yield is usually reported for a specific energy, such as 662
keV (137 Cs), 835 keV (54 Mn), or 1.836 MeV (88 Y), although in some cases a multitude of gamma-ray
energies may have been used for the calibration (see for example [Holl et al. 1988]). For statistical reasons,
a high absolute light yield is desirable for good gamma-ray energy resolution. In other words, the brighter
the scintillator, the better the energy resolution. The absolute light yields of several common inorganic
scintillators are listed in Table 13.1.
The relative light yield is the number of photons emitted per unit energy at different energies, reported
as normalized at a specific energy. Recent publications have used energies near 450 keV as the normalization
energy [Mengesha et al. 1998, Swiderski et al. 2009a, Payne et al. 2011]. The relative light yield is a measure
of the fluorescent response linearity to absorbed energy. Ideally, the relative light yield should be constant;
however, several physical factors can affect the light yield of scintillators, especially in the lower energy region
below 500 keV [Jaffe et al. 2007].
Although the cause of non-linear light yield is not fully understood, progress has been made in recent years
with predictive modeling. Discussions on different models that elucidate the non-linearity of light emission
can be found in the literature [Payne et al. 2009, Payne et al. 2011, Moses et al. 2012]. An important factor
affecting non-proportionality is the ionization density produced by an interacting charged particle (electron).
From the Bethe-Bloche expression for electron energy loss in matter (see Chapter 4), the ionization density
increases as the electron velocity (or energy) decreases. For most scintillators, there is a notable decrease in
relative light yield in the low energy region, as shown in Fig. 13.4 and Fig. 13.5, which indicates that light
yield for these scintillators decreases as ionization density increases. However, for several alkali-metal/halogen
scintillators, there is a notable decrease in light yield also in the high energy region (see Fig. 13.4), an
indication that the relative light yield is decreasing for low ionization densities. This ionization density is
dependent upon the initial excitation energy of the ejected electron produced by Compton scattering, pair
production, or the photoelectric effect. Further, the deexcitation processes, radiative or non-radiative, are
also dependent on the incident particle energy. Over the past several decades, there have been numerous
models proposed to predict or explain the relative light yield of inorganic scintillators, three of which are
described here [Moses et al. 2012].
The “minimalist model” uses numerous simplifying assumptions to arrive at a manageable model. Fore-
most, it is assumed that luminous emissions are produced solely from exciton recombination at luminous
defect centers. Further, it is assumed that free electrons and holes do not contribute to light emissions,

8 Also known as GOS or Gadox.


492 Scintillation Detectors and Materials Chap. 13

1.5 1.05
1.4

1.3 ideal
1.00 performance
1.2
Electron Response

Electron Response
(relative light yield)

(relative light yield)


1.1
0.95
ideal
1.0
performance
0.9
CsI(Na) 0.90
0.8
CsI(Tl)
NaI(Tl)
(relative light yield)

0.7
BGO SrI2(Eu)
0.6 CaF2 0.85 LaBr2(Ce)
LSO(Ce) LaCl2(Ce)
0.5
YAP LuAG(Pr)
0.4 0.80
1 10 100 1000 10 100

Electron Energy (keV) Electron Energy (keV)

Figure 13.4. Relative light yield for several inorganic scin- Figure 13.5. Relative light yield for several inorganic
tillating materials, all normalized at 440 keV. Data are from scintillating materials, normalized at 450 keV. Data are
[Mengesha et al. 1998]. from [Swiderski et al. 2009a, Payne et al. 2011].

but instead recombine non-radiatively. It would, therefore, be the loss of excitons to competing processes
that causes a reduction in relative light yield. The minimalist model seeks to explain this phenomenon as
losses due to collisions between excitons in which one exciton pair is changed into an electron-hole pair that
de-excites by non-radiative transitions but the other is ultimately preserved. The probability of this event
increases with the square of the charge carrier density and, hence, becomes dominant for low energy photon
interactions. Also assumed is that at higher energies, the electron and hole densities are less and are also
spatially separated. Only those electrons and holes within the Onsager radius RO can form mobile excitons.9
Based on the non-linear behavior described by Birks [1964], the light yield thus becomes,

dE/dx
1 − ηeh exp −
(dE/dx)RO
L= , (13.20)
dE
1 + kB
dx
where ηeh is the fraction of electrons and holes that do not form excitons, (dE/dx)O is the energy loss
where the average spatial separation between electrons and holes is RO , and kB is the quenching parameter
described by Birks [1964]. Payne et al. [2011] successfully apply Eq. (13.20) to effectively model the response
of numerous scintillator materials. Unfortunately, the minimalist model fails to predict relative light yield
from first principles, and is more akin to an empirical data curve fitting method.
The “kinetic model” includes phenomena that are known to occur and affect scintillation yield, but are
disregarded in the minimalist model. These effects include radiative emission from trap assisted electron-hole
recombination and the reduction of charge carrier density as recombination progresses. Through either a
rigorous system of mathematical rate equations, or through Monte-Carlo techniques, these kinetic models
attempt to track changes in the electron-hole-exciton cloud as a function of time. The analytical techniques
can be complicated, and attempt to include all processes that affect scintillation light yield. The stated
advantage is that this modeling method provides much insight into the scintillation mechanism of a material.
The disadvantage is the complexity involved with the model.

9 The Onsager radius RO is the physical distance between an electron and hole at which the electro-static energy is equal to
the thermal energy, i.e., q 2 /(RO ) = kT , where  is the dielectric constant and q is the unit electronic charge. At R < RO ,
the electron (or hole) cannot escape from the Coulombic force field. [Payne et al. 2009].
Sec. 13.2. Inorganic Scintillators 493

Figure 13.6. Measured light yield from several common scintillators compared to pre-
dicted results from a transport model. The responses are shown as functions of diffusion
coefficients. The term (1 - QF) is the fraction of carriers that survive at least 10 ps after
the charge cloud is formed. CdTe and HPGe are semiconductors, and the measured
metric is the charge carrier collection efficiency. Data are from [Li et al. 2011].

The “diffusion model” includes the effect of electron and hole mobility, as well as ambipolar diffusion
of excitons. Electrostatic forces and thermal diffusion affect the density of electrons and hole in a charge
cloud. Recombination is a strong function of the product np and the trap density (covered in Chapter 15). As
electrons and holes separate from diffusion, the probability of direct or trap assisted recombination decreases.
Excitons are treated as neutral particles, affected only by thermal diffusion. The overall result can be used
to modify the kinetic model. This carrier transport method has at least three major implications [Moses et
al. 2012]. First, if one charge carrier type diffuses much faster than the other, for instance μe μh , then
these differing charge carriers become physically separated and, thus, significantly decreases recombination.
Second, for materials with similar electron and hole diffusion coefficients, electrons and holes diffuse with
similar spatial distributions, thereby producing a high light yield by efficient recombination. Third, charge
carriers (and excitons) with high mobilities rapidly separate, thereby diminishing the carrier density and
reducing light loss from quenching. Consequently, it is expected that scintillation materials with relatively
high charge carrier mobilities have proportional light output, while the opposite is true for materials with
low charge carrier mobilities. The diffusion model has been successfully used to predict luminosity from
several common scintillators [Li et al. 2011] as shown in Fig. 13.6.
A scintillator is said to have a linear response if the light yield scales as

N  = kE + b (13.21)

where N  is the mean number of information carriers, E is the absorbed radiation energy, k is a propor-
tionality constant, and b is a constant. For the case of scintillators, N  is the average number of photons
produced per event at energy E. In such a case, the scaling of a scintillator is predictable, but the average
energy needed to produce a photon is a function of energy and is not constant (w = E/N  = constant). If
494 Scintillation Detectors and Materials Chap. 13

the constant b is zero, the scintillator is said to have a proportional response, in which case w = E/N  =
constant. Regardless of the value of b, the differential change in information carriers per differential change
in energy is constant, or dN /dE = 1/k = constant for both linear and proportional responses.
Non-linear (or non-proportional) light yield response as a function of energy complicates energy cali-
bration [Jaffe et al. 2007]. Ideally, the relative light yield (photons/MeV) should be constant, or at least
proportional, for all energies. Consequently, pulse height spectral features do not appear in channels pre-
dicted with a linear formula. For instance, the relative light yield for NaI deviates from 1 (at 662 keV) to
1.25 (at 10 keV), whereas YAP has minimal deviation in relative light yield as shown in Fig. 13.4. With
predictive modeling, a calibration can be developed to provide a reasonably accurate scaled response.

Example 13.1: You are using a NaI:Tl scintillator to measure gamma rays from different sources having
energies of 59.5 keV and 662 keV. If system gain puts the 662 keV gamma ray at channel 1000, in what
channel does the 59.5 keV gamma-ray center appear? Which channel should it appear in if the relative light
yield was constant at all energies?

Solution:
Although the 59.5-keV gamma ray is lower in energy than the 662-keV gamma ray, it produces more
light per unit energy. From Fig. 13.4, the relative light yield at 60 keV is about 1.15. To find the energy per
channel:
E/Ch = 662 keV/1000 = 0.662 keV/channel.

The channel in which the 59.5-keV gamma ray appears, corrected for the increase in light yield from 1.00
to 1.15,
Ch = (1.15)(59.5 keV)/(0.662 keV/ch) = channel 104.

rounded to the nearest channel. The 59.5-keV gamma ray should appear in channel 90 if the relative light
yield was constant.

Large deviations in relative light yield as a function of energy also adversely affect the energy resolution
by causing further statistical spread in the photon yield [Valentine et al. 1998]. Two factors identified by
Valentine et al. that contribute to energy resolution broadening are (1) multiple interaction events resulting
in one or more energetic primary electrons prior to photoelectric absorption and (2) the resulting electron
cascade sequence that follows photoelectric absorption which produces Auger electrons and x-ray emissions.
For instance, gamma rays of energy near 662 keV interact most often by Compton scattering in a medium
and, hence, deposit only a fraction of their energy in the scintillator at a Compton scatter location. For each
subsequent interaction, be it another Compton scatter event or photoelectric absorption, a different amount
of energy is deposited in the scintillator until either the photon is absorbed through the photoelectric effect
or the photon escapes the detector. Multiple events occur as the empty energy states created by Compton
scattering of photoelectric absorption are filled, which includes a cascade of Auger electrons and x-ray
emissions. These emissions can also be re-absorbed in the scintillation material. The overall light yield is the
sum from all of these events, starting from the initial Compton scatter interaction, all of which produce an
energetic electron of different initial energy. Because these energetic initial electrons are of different energies,
they also produce a different relative light yield. The variance in light yield about the average light produced
from this process must be added to the statistical variance in the average number of electron-hole pairs
(and excitons) produced. For ideally proportional scintillators, this variance contribution to the light yield
reduces to zero, although the fluctuations in the number of charges created from Poisson statistics remains.
Sec. 13.2. Inorganic Scintillators 495

Example 13.2: You are using a NaI:Tl scintillator to measure gamma rays from 137 Cs with gamma-ray
emissions of 662 keV. Suppose that one gamma ray undergoes photoelectric absorption ejecting a photoelec-
tron from the K shell of iodine. A second gamma ray produces a Compton electron of 150 keV, a second
Compton electron of 200 keV, and is then captured by the photoelectric effect. Determine the difference in
relative light yield and absolute light yield for these two events.

Solution:
The K-shell binding energy of iodine is 33.164 keV. Therefore, the first photoelectron is ejected with an
energy of
662 keV − 33.164 keV = 628.84 keV.
From Fig. 13.4, the relative light yield for the first gamma-ray absorption correlates to a relative light yield
of 1.0.
The remaining energy is preserved by numerous cascades of electrons through atomic energy levels,
but assume, to a first approximation, that a characteristic x ray from a KαI emission is produced, which
subsequently ejects a LII electron. Note that a variety of transitions are possible, but the differences in
these energy transitions are small. Hence,

28.61 keV(at KαI ) − 4.856 keV(binding energy at LII ) = 23.75 keV.

From Fig. 13.4, the relative light yield for the 23.75-keV Auger electron is about 1.2. The remaining energy
(approximately 9.41 keV) is absorbed through various Auger electron transitions. Because two L electrons
are missing, two allowed transitions from the M shell are chosen, namely Lα1 and the Lβ1 . Auger electrons
can be produced if these x rays are absorbed by the M shell. There are numerous possibilities, but we choose
MII or MIII electrons, then free electrons of energy 3.06 keV and 3.29 keV, respectively. From Fig. 13.4,
these emissions would produce a relative light yield of approximately 1.15 each. The remaining 3.06 keV
energy is regained by electrons relaxing into the M shell, producing free electrons with energies on the order
of 0.50 keV to 0.88 keV. Regardless of the transitions, extrapolation from Fig. 13.4 gives a relative light
yield near 1.0. If the relative light yield is tabulated in terms of fractions, then
628.64 keV 23.75 keV 3.06 keV + 3.29 keV 3.06 keV
RLY = (1.0) + (1.2) + (1.15) + (1.0) = 1.0083.
662 keV 662 keV 662 keV 662 keV
The expected absolute light yield is,
 
1 MeV
43, 000 photons/MeV (662 keV)(1.0083) = 28, 702 photons.
1000 keV

The same analysis can be done for the Compton scattered photons. The main difference is the ejection
of a 150-keV Compton electron (relative light yield of 1.06), a 200-keV Compton electron (relative light
yield of 1.03), and the subsequent absorption of the 312-keV Compton scattering photon, which produces
a 278.8-keV photoelectron (relative light yield of 1.01). With a similar Auger electron cascade scheme, one
arrives at the total relative light yield of 1.0345. The expected absolute light yield is,
 
1 MeV
43, 000 photons/MeV (662 keV)(1.0345) = 29, 448 photons.
1000 keV

The total percent difference between the single photoelectric absorption and the Compton scattered example
is
1.0345 − 1.0083
(100) = 2.6%.
1.0083
496 Scintillation Detectors and Materials Chap. 13

Decay Time and Pulse Formation


Suppose a radiation particle interacts in a material and excites N ∗ electron-hole pairs. Of these N ∗ electrons,
an average fraction of electrons fall into luminescent centers, represented by N = f N ∗ . The rate at which
these free electrons fall into luminescent centers can be represented as a decay rate,

dN (t) N (t)
= −λr N (t) = − , (13.22)
dt τr
where N (t) is the population of free electrons that eventually fall into luminescent centers, λr is the prob-
ability, per unit differential time, that an electron falls into a luminescent center from its mobile state and
τr is the mean decay time in which the subscript r designates ‘rise’. The rate at which electrons, once in
luminescent centers, decay and release a photon is given by
dNc (t) Nc (t)
= −λd Nc (t) = − , (13.23)
dt τd
where λd is the probability, per unit differential time, that an electron falls into a luminescent center from
its mobile state and τd is the mean decay time. Here the subscript d designates ‘decay’. Hence, the rate of
change in luminescent center population, immediately after a radiation interaction event, is
dNc (t) N (t) Nc (t)
= − . (13.24)
dt τr τd
From the solution of this equation, the luminescent center population immediately after a radiation interac-
tion is,
τd
Nc (t) = N e−t/τr − e−t/τd . (13.25)
τr − τd
The light emission rate, in photons per unit time, is expressed as a function of the decay time,
Nc (t) N
L(t) = = e−t/τr − e−t/τd . (13.26)
τd τr − τd
Note that if the population ‘rise time’ is extremely short (≤ a few ns), which it usually is, then Eq. (13.26)
reduces to,
N −t/τd
L(t)  e . (13.27)
τd
The solution of Eq. (13.26) is derived with the assumption that a single decay time can adequately represent
the light emission rate of a scintillation material. The decay times listed in Table 13.1 are average values
obtained from an experiment. Many luminescent states may play a part in the emission sequence. Often
these decay times for separate energy levels are similar enough that an average decay time adequately defines
the light emission behavior. However, there are many scintillators that have multiple decay times that are
notably different. Some also have different emission wavelengths. As seen from Table 13.1, CsI:Na, CsI:Tl,
and BaF2 are examples of scintillators with multiple decay times. In fact, there is a significant difference in
the decay times and the maximum wavelengths λmax for BaF2 emissions.
Differences in decay time constants can be used to distinguish between particles, energies, and in some
circumstances the particle mass. One example is the phoswich10 detector, where two different scintillators
with different time constants are laid one upon the other, and read out by a single light detection device.
By distinguishing between the times constants, the operator can discern in which detector the interactions
occurred. Designs and uses of this configuration are discussed in Chapter 20.

10 Phosphor sandwich.
Sec. 13.2. Inorganic Scintillators 497

Energy Resolution
The energy resolution of a radiation spectrometer is defined as the full width of the spectroscopic energy
peak (usually ΔE) at half the maximum intensity (FWHM). The energy resolution from scintillators is
traditionally reported in terms of percent of the most probable energy (the mode) in the pulse height
spectrum,  
FWHM
R% = 100 . (13.28)
Emax
The minimum value of the FWHM can be modeled, to a first approximation, with Poisson statistics, i.e.

FWHM = 2 2 ln(2)var(E), (13.29)

where var(E) is the variance of the full energy peak in the pulse height spectrum. A FWHM is depicted in
the example gamma-ray pulse height spectrum of Fig. 6.18, taken with a NaI:Tl detector. If the scintillator
is coupled with a PMT light detector (Ch. 14), the light collected is converted to an electron signal. Hence,
with the assumption that electronic noise from other electronic components is minimal, the variance in
the number of electrons
 collected by the PMT is a measure of the variance of the pulse height spectrum,
or var(E)/Emax ≈ var(Q)/Qmax . The fractional variance in electrons collected by the PMT can be
expressed as [Birks 1964]

var(Q) var(N ) 1 var(p) Ḡ2 + var(G)


v(Q) = ≈ − + + , (13.30)
Q̄ 2 N̄ 2 N̄ p̄2 Ḡ2 N̄ p̄

where var(N ) is the variance in the number of scintillation photons, N̄ is the average number of scintillation
photons, var(p) is the transfer variance, p̄ is the average transfer efficiency, Ḡ is the PMT gain, and var(G) is
the variance in the PMT gain (an intrinsic characteristic of the PMT). The transfer efficiency, and associated
variance, are factors that affect the efficiency of how well photons produce photoelectrons, which may include
scintillation wavelength matching to the PMT response, coupling efficiency between the scintillator and the
PMT window, internal reflection, index of refraction mismatch between the scintillator and the PMT window,
photocathode nonuniformities, and photoelectron collection efficiency [Dorenbos et al. 1995].11 For the case
of scintillation light yield based on Poisson statistics, the variance and the average value are equal, i.e.,

var(N ) = N̄, (13.31)

and the bracketed expression in Eq. (13.30) reduces to zero. However, there are other intrinsic factors
that can affect the energy resolution. The main two factors are (1) non-proportional light yield, discussed
previously, and (2) non-uniformities in the luminescent center (activators) distribution. The overall energy
resolution measured from the scintillator detectors becomes,

R2 = Ri2 + Rp2 + RG
2
(13.32)

where Ri is the intrinsic light yield resolution of the scintillation crystal, Rp is the transfer resolution, and RG
is the PMT limiting resolution. Although there are methods to independently measure the effects of Ri and
Rp , these contributions to the energy resolution are often combined and defined as the detector resolution
Rd2 = Ri2 + Rp2 . For an ideal detector perfectly coupled to a PMT, Rd = 0 and p̄ = 1; hence Eq. (13.30)
reduces to,
1 + var(G)/Ḡ2
v(Q) ≈ . (13.33)

11 These factors affecting PMT performance are explained in Chapter 14.
498 Scintillation Detectors and Materials Chap. 13

Figure 13.8. The light output, normalized at the maxi-


mum for τ = 1μs, as a function of temperature for several
common inorganic scintillators. The light output data for
Figure 13.7. Measured energy resolution for several inor-
NaI:Tl, BGO, and LaCl3 were normalized for data measured
ganic scintillating materials. Also shown is the theoretical
with a 1 μs shaping time, and comparison data is provided
limiting energy resolution. Data are from [Dorenbos 2002].
at longer shaping times. Data are from [Lindow et al. 1978,
Saint-Gobain 2016].

Values for var(G)/Ḡ2 are usually between 0.1 to 0.2 [Dorenbos et al. 2002]. Hence, the ideal best energy
resolution of a scintillator as a function of the number of photoelectrons produced becomes,
 
 1 + 0.1 1 + 0.1
% FWHM ≈ 2 2 ln(2) = 2.355 . (13.34)
N̄ N̄
This ideal energy resolution is plotted as a solid line in Fig. 13.7, and is compared to measured values of many
common inorganic scintillators. From Fig. 13.7, it is clear that almost all of the scintillators represented fall
short of the predicted ideal energy resolution. Factors that broaden the energy resolution limit include non-
proportional light yield, poor reflective properties of the crystal encapsulate, crystal transparency, crystal
imperfections, and mismatch between the indices of refraction at the scintillator and light collection window
interface. It is noteworthy that many of those scintillators shown to have large deviations from the predicted
resolution also have significantly non-proportional light yield in the low energy region (< 200 keV), an
indication of the importance of proportional light yield on scintillator performance. Energy resolution can
sometimes be improved with better crystal synthesis and production methods. For instance, the energy
resolution of the material YAlO3 :Ce (YAP) was reportedly reduced from 6% to 4.4% by improving the
crystals (compare results of [Kapusta et al. 1999] to [Moszynski et al. 1998]).
Thermal Properties
From Fig. 13.2 and the explanation offered in the section on emission spectra, scintillation light yield at high
temperatures (> 100◦C) generally result in a reduction in relative light yield. One cause of the reduction is
the increased numbers of excited electrons lost from direct transfer from the excited state to the ground state
[Melcher 1989]. Another source of a decrease in light yield is the increase in σe (T ) with increasing temperature
as can be seen from Eq. (13.14). This increase in σe (T ) spreads the light emission over more wavelengths
and, consequently, reduces the maximum yield at λmax . This reduction increases photon reabsorption from
crystal defects as a result of increased wavelength mismatch between the light emissions and the light sensor
(PMT, photodiode, etc.).
Sec. 13.2. Inorganic Scintillators 499

There is also a notable decrease in light yield for many scintillators at low temperatures, particularly at
temperatures below room temperature. This decrease in relative light yield can be explained, at least in
some circumstances, as a consequence of lengthening the primary decay constant. If the time constant of a
light sensor is not lengthened to match the relative increase in τ , then an increased number of luminescent
photons are not recorded. From Fig. 13.8, the light output of many common scintillators appears to decrease
with lower temperature; however, changing the integration time of the light sensing system works to include
previously lost photons, thereby increasing the relative light yield. Examples of such scintillators include
BGO (1 μs → 12 μs), NaI:Tl (1 μs → 12 μs), and LaCl3 (1 μs → 16 μs). Scintillators that have relatively
flat thermal response to light yield over a broad range of energies include LaBr3 and BaF2 (220 nm emission
only).
Material and Optical Properties
Important material properties for scintillators include fracture resistance, atomic number, mass density,
radiation absorption length, and moisture resistance. The atomic number and material density affect the
radiation absorption length. For gamma-ray detection, materials with at least one high Z component are
best. Further, a high atomic density of the high Z constituent assists with photon absorption. For this
fundamental reason, scintillators with high Z are sought for a variety of gamma-ray detection applications,
including medical imaging, oil well logging, and gamma-ray spectroscopy. However, because of backscattering
effects, low Z materials are best used for alpha-particle and beta-particle detection, and scintillators in which
all constituents are low Z are best applied.
The fracture resistance is a measure of a scintillation crystal’s ability to withstand shock. Many of the
alkali-metal/halide and lanthanide/halide scintillators are soft and extremely fragile and crack under modest
exposure to shock. For instance, NaI and CsI are both listed as ‘2’ on the Moh hardness scale,12 an indicator
of resistance to fracture and plastic deformation. NaI is fragile and cracks easily, while CsI is pliable and can
withstand more shock. Packaging improvements, which have internal shock resistant buffer regions, have
allowed many of these delicate crystals to be used in rough environments such as oil well logging. Oxide based
scintillators tend to be more resilient to shock than alkali halides, and they offer a solution for measurements
conducted in rough environments. Some oxide based scintillators have high Moh hardness values, such as
YAG (moh = 8.5) and YAP (moh = 8.6).
Many of the alkali-metal/halide and lanthanide/halide are chemically unstable in a humid environment,
and require handling in special ‘dry rooms’ during the cutting and packaging process. Further, these hygro-
scopic crystals must be hermetically sealed in air tight containers to prevent decomposition. Otherwise they
may absorb water moisture, which causes them to change color and/or decompose. The alkali-metal/halides
NaI:Tl and LiI:Eu are very hygroscopic and are ruined if exposed to humidity. The same is true for the lan-
thanide/halides LaBr3 :Ce, LaCl3 :Ce, and CeBr3 . CsI:Na is also hygroscopic; however, pure CsI and CsI:Tl
are only slightly hygroscopic. Oxide-based scintillators along with the alkali-earth/halides generally are not
hygroscopic.
Two important optical properties are crystal clarity and the index of refraction, both at the scintillator
peak luminescent wavelength. The scintillator materials should be transparent to the photons emitted by
the luminescent centers; otherwise, they are reabsorbed and remain undetectable. The optical attenuation
coefficient is defined as α = 1/d, where d is the distance that a packet of photons with wavelength λ reaches
an absorption loss of 1−e−1 (63.21%). A large Stokes shift assists with optical clarity, in that the luminescent
photons are less likely to be absorbed in the crystal. The index of refraction is the ratio of light speed in
vacuum to light speed in the medium (n = c/v). As presented in Chapter 14, this ratio changes with light

12 This hardness scale, still used today, was initially developed in 1812 by Frederich Moh, who compared materials to ten
commonly available minerals used as standards. The scale ranges from 1 to 10, with talc rated as ‘1’ and diamond as ‘10’. It
is neither linear nor logarithmic, but is ordinal and somewhat arbitrary in designation.
500 Scintillation Detectors and Materials Chap. 13

VK-center H-center R-center


- - - - - - -

+
- - - - - -

+
- - h+ - - - -
e-

+
- h+
+ e- - - - e- e-

+
- + e- - - - - -

+
e-
- - - e- -
+

+
e-
- - - - - - -
+

+
M-center F’-center F-center

Figure 13.9. Depiction of several types of defects that can


be formed in a crystal. F , F  , M , and R centers involve
vacancies, whereas VK and H centers do not.

wavelength; hence the important value is the index of refraction at the most probable emission wavelength
λmax . This index of refraction should be as close as possible to that of the light sensing instrument to obtain
good coupling and light transmission. For typical glass windows on light sensing instruments, a scintillator
index of refraction ≤ 1.5 is best.

Radiation Hardness
Radiation hardness is a relative measure of how well a substance resists changes in its important properties
when exposed to large radiation doses. For scintillators, radiation hardness is usually used to describe
the overall resistance to changes in its photon yield, pertaining either to luminescent intensity or emission
spectra. Absorption of radiation causes changes in the crystalline structure, which can cause the introduction
of defect centers called color centers. When a crystal takes on a visible hue, it has color centers in its makeup.
These colors centers can absorb the scintillation light and re-emit light at a different wavelength.
Although there are many types of color centers, perhaps one of the best under-
stood is the F -center, so called from the German Farbzentrum, translated “color
center”. An F -center is formed by the displacement of a negative ion in the crys-
tal structure, forming an anionic vacancy, which can trap an electron. The defect
is formed by the coupling of a positive acting vacancy and the negative electron.
S This vacancy-electron combination produces energy levels in the band gap of the
crystal, which can reabsorb luminescent photons, and through the Stokes shift,
re-emit them at longer wavelengths, or lose the excited electron by phonon inter-
F actions. The net effect is to reduce the light yield. F -centers are native defects
in alkali halide crystals, but can also be formed by x-ray, electron, or gamma-ray
irradiation. In some cases, F -centers can be removed or reduced by annealing
the crystal. There are many variants of these F -centers, all based on additional
S
defects coupled to an F -center [Kittel 1956]. Included in the list of F -center
variants are F  -centers, R-centers, and M -centers [Singh 2012], although the F -
center is the most common. An F  -center is an anion vacancy with two trapped
Figure 13.10. Depiction of electrons [Kittel 1956], an M -center is a formation of two localized F -centers, and
a Frenkel pair and a Schottky an R-center is a formation of three localized F -centers (see Fig. 13.9).
defect pair (vacancies). Trapped hole defects can also be formed, but do not involve a cation vacancy.
Instead, a trapped hole is associated with either one or more negative ions [Ashcroft and Mermin 1976].
A Vk -center is formed when a hole is bound to two neighboring negative ions in the crystal, producing
Sec. 13.2. Inorganic Scintillators 501

characteristics of a singly charged negative diatomic ion (A−


2 ). The H-center is formed when a hole is bound
to both an interstitial anion and neighboring anion in the lattice, forming a singly charged negative diatomic
ion at the ion lattice location.
With sufficient energy transfer, lattice atoms can be removed from their respective sites into interstitial
locations. If the removed ion is a cation, creating a positive ion interstitial in the crystal and leaving
behind a negatively charged vacancy, a Frenkel defect is formed, consisting of the vacancy-interstitial pair
(see Fig. 13.10). If a negative ion vacancy is formed along with a positive ion vacancy, the defect pair is a
Schottky defect. By definition, a Schottky defect is not paired with interstitial ions, the Schottky defect pair
maintaining electrical neutrality and crystal stoichiometry. Hence, Schottky defects are more likely formed
near surfaces where the displaced ions can leave the crystal bulk.
The energy required to displace atoms in most solids is on the order of 25 eV. Hence, energy transfer in
excess of 25 eV by radiation interactions can lead to the formation of both Frenkel and Schottky defects.
Gamma-ray irradiation can form Frenkel (and Schottky) defects by transferring energy to electrons, through
photoelectric, Compton scattering, or pair production interactions, which in turn transfers kinetic energy to
lattice atoms.
A single energetic neutron can transfer enough energy to a recoil atom that can subsequently cause a
cascade of displacements, forming a void in the crystal. The maximum energy transfer from a radiation
particle to a lattice atom is given by Eq. (4.58), repeated here for convenience,
 
β2 2M m2i c2
Tmax =  .
1 − β 2 m2i + M 2 + [2mi M/ 1 − β 2 ]

where M is the target atom mass, mi is the radiation particle mass, β = vi /c is the velocity ratio of mi ,
and c is the speed of light. The magnitude of Tmax must be greater than the displacement energy in order
to produce these radiation-induced defects. For non-relativistic particles, Eq. (4.58) reduces to
mi M
Tmax ≈ 4E . (13.35)
(mi + M )2
These radiation-induced traps can form color centers, as well as shallow and deep electron and hole traps.
Irradiation with hadrons13 can cause activation and autodoping. Activated crystals possess intrinsic
background radiation that is present during radiation measurements. Autodoping is a process in which
constituent atoms are transmuted into different elements, thereby producing new activator sites (energy
levels). It is possible that these newly formed energy levels reduce light yield by quenching the light emissions
from luminescent centers.
The main effect of radiation induced defects, the most common of which are color centers, is to reduce
the light emission from the scintillator. However, many of these defects heal over a relatively short time,
thereby allowing the scintillation crystal to recover. Alkali halide scintillators tend to be more susceptible
to hadron damage than photon (or electron) induced damage, while oxide-based scintillators tend to suffer
more damage by photons than do alkali halides [Rodnyi 1997]. However, the extent of damage from radiation
exposure depends on the type of crystal and the type of radiation. A study by Zhu [1998] on several
common scintillators indicated that oxygen contamination in the alkali halides was the main source of
radiation damage in these scintillators. Apparently the incorporation of hydroxyl groups (OH− ) into a
scintillator can be broken down by radiation interactions in the crystals, after which the constituents migrate
to become interstitials or substitutional atoms in the crystalline lattice [Zhu 1994]. Work performed by Zhu

13 Hadrons are categorized as either baryons or mesons. Baryons have three quarks and include neutrons and protons. Mesons
have one quark and one antiquark and include pions and kaons.
502 Scintillation Detectors and Materials Chap. 13

[1996] provides evidence to support this theory who showed the radiation hardness of CsI:Tl was improved
by reducing the oxygen contamination. Zhu [1998] also concluded that radiation damage to oxide-based
scintillators was due mainly to the formation of oxygen vacancies.
Ishii and Kobayashi [1991] studied the effects of gamma radi-
ation on scintillator performance. The study, conducted for ap-
plications in high energy physics, defined radiation hardness as
that dose at which the light transmittance decreased by 2% per
unit gamma-ray attenuation length (see Fig. 13.11). Although
this measure may not apply to all scintillator applications, it
does provide a relative measure of the radiation hardness be-
tween various common scintillator materials. From Fig. 13.11,
of those scintillators studied, NaI:Tl, CsI:Tl, cadmium tungstate
(CdWO4 ), and PbF2 had the lowest radiation resistance while
gadolinium orthosilicate (GSO) had the highest tolerance. Zhu
[1998] found that, depending on the dose rate, BGO and PbWO4
can quickly (hours to weeks) recover from radiation damage at
room temperature. Some of the more interesting properties re-
Figure 13.11. The radiation hardness of sev-
eral scintillators versus unit radiation absorption
garding radiation hardness are described for a few specific scin-
length. Data are from Ishii and Kobayashi [1991]. tillators in the following sections.

13.2.3 Properties of Several Common Inorganic Scintillators


Scintillators have been used for various radiation detection applications for over a century. Fluorescent
screens and coatings were used in Crookes tubes, and PtBa(CN)4 was the scintillating material that led
to Röntgen’s discovery of the x ray. ZnS:Ag was used for alpha particle counting by Rutherford, Geiger,
and Crookes. In the early 1940s, organic scintillators were matched with efficient light collection devices to
produce better scintillation detectors. However, it was the discovery of the bright inorganic scintillator NaI:Tl
in 1948 by Hofstadter that allowed the practical application of scintillators to gamma-ray spectroscopy. Since
then, the search has continued for better and brighter scintillators for higher energy resolution gamma-ray
spectroscopy.
There have been some limited successes, which include those scintillators listed in Table 13.1. For instance,
CsI:Na is similar in performance to NaI:Tl, but has a longer decay time. CsI:Tl has much higher light output
than NaI:Tl, but the emission spectrum has a maximum at 560 nm, a wavelength that does not couple well
to PMTs. However, CsI:Tl has been coupled to Si photodiode sensors quite successfully. Bismuth germanate
(BGO) has lower light output, but is much denser and a better absorber of gamma rays. As a result, BGO
has been used for medical imaging systems to reduce the overall radiation dose that a patient receives during
the imaging procedure. In recent years, LSO:Ce has become an effective and useful alternative to BGO.
LSO:Ce has higher light yield than BGO while also having comparable gamma-ray sensitivity. LiI:Eu is a
scintillator that is primarily used for neutron detection because of the 6 Li content in the crystal. In recent
years, LaBr3 :Ce, a relatively new scintillator with exceptional properties for gamma-ray spectroscopy, has
become available. LaBr3 :Ce has a much higher light yield and a much shorter decay time constant than
NaI:Tl. Further, it is composed of higher Z elements and, hence, is a better gamma-ray absorber than NaI:Tl.
However, it is extremely hygroscopic and fragile and, thus, it is difficult to produce and handle. Although it
has become commercially available, it is presently much more expensive than NaI:Tl because of production
and fabrication problems.
Overall, there are numerous inorganic scintillators available for special radiation detection purposes. In
fact, after more than 120 years of exploration for different scintillators, several hundreds have been identified.
For example, tables of scintillators numbering in the hundreds, still incomplete, can be found in the literature
Sec. 13.2. Inorganic Scintillators 503

[Derenzo et al. 1991, 2016]. It is beyond the scope of the present text to be all inclusive of this extensive list
of scintillators, and the authors limit the following descriptions to those scintillators that either have proven
applications, historical significance, or show potential as scintillators for new applications.

Alkali-Metal Halide Scintillators


This family of scintillating salts composed of alkali metals and halogens is perhaps the most successful class
of bright scintillators. Outlined here are some properties of a few notable scintillators in popular use, which
are also listed in Table 13.1. A convenient and more extensive list of scintillator properties is provided by
Derenzo et al. [2016].

Sodium Iodide (NaI, NaI:Tl) The most widely used inorganic scintillator is NaI:Tl. The notation ‘:Tl’
indicates that the NaI crystal has been doped with the activator Tl. It is one of the brightest scintillators
available, has acceptably good light yield proportionality, and can be grown in large sections. NaI:Tl was
first reported by Hofstadter [1948] who prepared, initially, a powder sample of material with thallium added
to the mixture that produced scintillation light when exposed to alpha particles. The sample was found to
be hygroscopic, turning yellow within a few hours when exposed to room air. He then produced tiny NaI:Tl
crystals (about 1 to 2 mm in size) in an evacuated ampoule. These crystals proved to be brighter than other
scintillating materials known at the time.
NaI:Tl yields approximately 43,000 photons
per MeV of energy absorbed in the crystal.
Light emitted from NaI:Tl has a continuous
wavelength spectrum, with a most probable
emission at λmax = 415 nm. The emission
spectrum from NaI:Tl matches well to com-
mon K-bialkali and S-11 commercial photomul-
tiplier tubes. NaI:Tl shows non-proportional
light yield in the low energy region, below 200
keV, which consequently compromises spectro-
scopic performance. Regardless, NaI:Tl per-
forms adequately well for a general use gamma-
ray spectrometer. The decay time for NaI:Tl
is 230 ns, which is relatively long compared to
almost all organic scintillators and some inor-
ganic scintillators. Although the decay time is
manageable, it generally precludes NaI:Tl as a Figure 13.12. Gamma-ray linear attenuation coefficients for sev-
candidate for fast timing measurements. eral common alkali-metal halide scintillators. Data are from [NIST
For the most probable wavelength of 415 nm XCOM].
(E = 2.99 eV), a photon yield of 43,000/MeV represents only 12.8% of the energy absorbed. Other mech-
anisms for energy relaxation include phonons (heat) and phosphorescence. NaI:Tl has a slow 150 ms phos-
phorescent component, contributing about 9% of the photoelectron yield [Koički et al. 1973]. The emission
rate is relatively low but usually does not interfere with low activity measurements, mainly because the low
emission rate of phosphorescence produces low pulse height events easily rejected by a discriminator. This
phosphorescent yield becomes important for high gamma-ray interaction rates during which it can become
a steady source of background noise for radiation measurements and is often called afterglow.
Yet, it is the availability of large sizes and the relative linear response to gamma rays that makes NaI:Tl
so important. Many different sizes are available, ranging in size from cylinders that are only 0.5 inches in
diameter to almost a meter in diameter. Yet, the most preferred detector geometry remains the 3 × 3 inch
504 Scintillation Detectors and Materials Chap. 13

right circular cylinder. It is the most characterized NaI:Tl detector size with extensive efficiency data in the
literature. Further, it is the standard by which all other inorganic scintillators are measured.
NaI:Tl is widely used to measure x rays
and gamma rays because of its high efficiency
for electromagnetic radiation, mainly due to
the high interaction efficiency of iodine (see
Fig. 13.12). The primary interaction efficiency
as a function of gamma-ray energy and detector
thickness is shown in Fig. 13.13.14 X-ray detec-
tors with a thin entrance window containing a
very thin NaI:Tl detector are often used to mea-
sure the intensity and/or spectrum of low energy
electromagnetic radiation. NaI:Tl detectors do
not require cooling during operation and can be
used in a great variety of applications. The bare
NaI:Tl crystal is hygroscopic and fragile. How-
ever, when properly packaged in ruggedized con-
tainers, field applications are made possible and
Figure 13.13. The calculated interaction efficiency for photons in
NaI:Tl detectors can operate over a long time
NaI as a function of energy and detector depth. The probability of period in warm and humid environments, resist
an initial interaction is shown and not the probability of subsequent a reasonable level of mechanical shock, and are
or multiple interactions. resistant to radiation damage. For any applica-
tion requiring a detector with a high gamma-ray efficiency and modest energy resolution, the NaI:Tl detector
is clearly a good choice.
Pure NaI also produces scintillation light without the assistance of activator dopants. At room tempera-
ture, the light yield of pure NaI is low, having less than 2% energy conversion efficiency with a most probably
emission wavelength of λmax around 310 nm [Van Sciver 1956; Van Sciver and Bogart 1958]. Relatively recent
measurements by Moszinzki et al. [2003b] with room temperature pure NaI indicated the release of 1,000
photoelectrons/MeV for a bialkali type PMT [Moszynski et al. 2003a]. The decay constant is substantially
smaller for pure NaI than for NaI:Tl, being less than 20 ns at room temperature. At cryogenic temperatures,
the light yield increases tremendously up to 25% energy conversion efficiency [Van Sciver and Bogart 1958],
a yield of about 63,000 photons per MeV with a maximum light emission at approximately 77 K. Recent
measurements put this yield for pure NaI closer to 44,000 ± 4,000 photons/MeV at 77 K [Moszynski et al.
2002]. Note that this trend of increased light yield with reducing temperature is observed for the entire
family of pure alkali-metal/iodine scintillators [Boananami and Rossel, 1952]. The decay constant τ for pure
NaI increases as the temperature is lowered, increasing from about 16 ns at room temperature up to about
95 ns at 4 K and about 63 ns at 77 K [Van Sciver and Bogart 1958].
The performance of pure NaI at low temperature (125 K), when coupled to a PMT, was reported as
18% FWHM for 122 keV gamma rays [Persyk et al. 1980]. As pointed out by Van Sciver and Bogart [1958],
there are problems with operating scintillators coupled to PMTs at low temperature, which include efficient
cooling of the PMT that is coupled to the scintillator, difficulties with coupling compounds that retain

14 Figures such as Fig. 13.13 have been used for decades in textbooks and commercial literature and have been labeled as
“absorption efficiency”. However, this designation is misleading, because these dependencies are generated from only the
total gamma-ray interaction coefficient μ by taking % “efficiency” as 100(1 − exp[−μt x]). The calculation does not take into
account Compton scatter losses or 511 keV losses from pair production, but instead represents only the probability of a primary
interaction occurring. High energy gamma rays are predominantly forward scattered, leading to reduced energy attenuation
and higher losses.
Sec. 13.2. Inorganic Scintillators 505

needed characteristics at cryogenic temperatures, and the fact the scintillators must be relatively small (<
12.5 mm thick) to reduce photon self-absorption losses. At least one of these problems can be addressed by
coupling pure NaI to a photodiode instead of a PMT, as reported by Moszynski et al. [2002; 2003a; 2003b].
This use of a photodiode gave 3.8 ± 0.1% FWHM for 662 keV gamma-rays when cooled to 100 K.

Cesium Iodide (CsI, CsI:Tl, CsI:Na) The absolute light yield of thallium doped CsI (CsI:Tl) has been
measured to have a range between 54,000 photons/MeV to 61,000 photons/MeV by various sources [Saint
Gobain 2016; de Haas et al. 2005; Mozynski et al. 1997b]. The refractive index is 1.79 and has a critical
angle of 56.9◦ with a glass interface. The material is only slightly hygroscopic and is much more resilient
than NaI:Tl. In fact, CsI:Tl can be machined
(to some extent) and it has significantly fewer
problems with shock and fracturing. Thin
sheets of CsI:Tl are slightly malleable and can
be formed over curved surfaces. With con-
stituent elements Cs (Z = 55) and I (Z = 53),
the gamma-ray attenuation coefficient is higher
than that of NaI:Tl, as shown in Fig. 13.12.
Hence, the gamma-ray intrinsic detection effi-
ciency per unit volume is better for CsI:Tl than
NaI:Tl. The primary interaction efficiency as
a function of gamma-ray energy and detector
thickness is shown in Fig. 13.14.
CsI:Tl has two decay components, 600 ns
and 3.5 μs, with λmax of 550 nm [Saint Gob-
ain 2016]. Although CsI:Tl has a considerably
higher light yield compared to most inorganic
Figure 13.14. The calculated interaction efficiency for photons in
scintillators, the large mismatch of the lumi- CsI as a function of energy and detector depth. The probability of
nescent spectrum with the response functions an initial interaction is shown and not the probability of subsequent
of common S-11 and K-bialkali PMTs, as can or multiple interactions.
be seen from Fig. 13.3, compromises the spectroscopic performance. The spectroscopic performance can be
improved by using long shaping times, thereby collecting more of the light from the luminescence. However,
a longer collection time increases dead time problems and integrates more electronic noise. The maximum
emission wavelength fortuitously matches well to the response function of Si photodiodes. Hence, reasonable
spectroscopic performance can be achieved by coupling CsI:Tl crystals to either Si photodiodes or Si photo-
multipliers (or SiPMs; see Chapter 14). The maximum light output of CsI:Tl is observed at approximately
50◦ C, and reduces with lower or higher temperatures (see Fig. 13.8). Temperatures deviating only ±50◦ C
from the optimum can cause a light yield reduction greater than 15%. Light loss to gamma radiation damage
can become significant at doses approaching 10 Gray, with a measured light reduction of 15% [Saint Gobain
2016].
CsI:Tl can be grown by physical vapor deposition to form narrow vertical columns of the crystal [Jing
et al. 1992]. Methods have been developed that create layer thicknesses up to 2 mm with column diameters
as small as 5 μm [Nagarkar et al. 1998]. These columns perform as miniature optical fibers that propagate
light, directionally, through the scintillator to the readout device. The CsI:Tl thin film can be patterned
through optical lithography methods to place the scintillator on select locations [Jing et al. 1992]. When
coupled to a Si diode or SiPM, the structure can be used to image a collimated beam of x rays. X-ray spatial
resolution on the order of 75 microns was reported when the device was exposed to a collimated 25 μm wide
≤ 30 keV x-ray beam [Jing et al. 1992].
506 Scintillation Detectors and Materials Chap. 13

A variant of CsI has Na as the activation dopant. The absolute light yield of CsI:Na has been measured to
range between 41,000 photons/MeV and 49,000 photons/MeV [Saint Gobain 2016; de Haas et al. 2005]. The
refractive index is 1.84 with a critical angle of 54.6◦ to a glass interface. CsI:Na is much more hygroscopic
than CsI:Tl, and care must be taken to prevent exposure to moisture. The primary decay time is also
long, but less than CsI:Tl at 630 ns, with a λmax of 420 nm. This luminescent spectrum from CsI:Na is
a much better match to common K-bialkali and S-11 PMTs (see Fig. 13.3), with a reported photoelectron
production about 85% of that observed with NaI:Tl [Saint Gobain 2016]. However, with the long decay time
and the lower resolution performance, CsI:Na offers little advantage over NaI:Tl, except, perhaps, for its
superior mechanical robustness. The maximum light output of CsI:Na is observed at approximately 80◦ C,
and reduces with temperatures either lower or higher (see Fig. 13.8). The thermal dependence is greater
than observed with CsI:Tl, and temperature deviation of ±50◦C from the optimum can cause a light yield
reduction greater than 20%.
Undoped CsI (or CsI(pure)) also produces scintillation light, but has very different properties than
activated CsI:Tl or CsI:Na scintillators. At room temperature, it produces approximately 2,000 photons
per MeV, with λmax at 315 nm [Saint Gobain 2016]. The index of refraction for pure CsI is 1.95, which
produces a critical angle of 50.3◦ at a glass interface. The primary decay time is much shorter than its doped
counterparts, namely about 16 ns. Amsler et al. [2002] conducted experiments to measure the light yield
and time response, and report the existence of three decay constants, all significantly shorter than doped
CsI, namely 28 ± 2 ns, 6 ± 1 ns, and a third fast component reported to be 2 ns. Notably, the light yield of
pure CsI increases significantly at low temperature, with a documented light yield of 50000 ± 5000 photons
per MeV at 77 K [Amsler et al. 2002] and yielded an energy resolution of 8.3% FWHM for 511 keV photons
when coupled to a PMT. Only a single decay constant was observed at low temperatures, which increased
significantly up to about 1 μs at 85 K.
Both pure CsI and CsI:Tl recovered from radiation damage at room temperature, but at a slow rate of
less than 0.5% per day. Thermal annealing of CsI or CsI:Tl does not assist with recovery, and appears to
make matters worse if conducted at temperatures exceeding 300◦ C.

Lithium Iodide (LiI:Tl, LiI:Eu) Lithium iodide is an alkali-metal halide scintillator that is used as both
a gamma-ray and neutron detector. LiI is hygroscopic and must not be exposed to humidity. Thus, LiI
requires all handling to be performed in a dry environment. LiI has been used as a scintillator for several
decades after being developed around the same time that NaI:Tl was introduced [Hofstadter 1948; Hofstadter
at al. 1951]. These initial LiI crystals were doped with Tl as the activator [Hofstadter 1950]. Many of these
crystals were yellowish in color, most likely a side effect from impurity contamination. It was also discovered
that the activator dopant distribution in LiI:Tl was non-uniform, a side effect from crystal growth problems.
The dopant source (LiTl) introduced into the crystal melt was not uniformly incorporated into the crystal
lattice, a result which consequently compromised the spectroscopic performance [Bernstein and Schardt
1952]. Within a few years, alternative activator dopants were studied including In, Ag, Sn, Sm, Eu. Of
these alternative activator dopants, Eu gave the best light output [Nicholson et al. 1955], and LiI:Eu remains
the most studied and used of the LiI variants. With a mass of 4.08 g cm−3 , LiI:Eu has nearly the same
gamma-ray interaction efficiency as NaI:Tl. LiI:Eu is a relatively slow scintillator with a decay time of 1.4
μs. The measured λmax value is 475 nm with an absolute photon yield of approximately 1,500 per MeV,
and has yielded 7.5% FWHM energy resolution for 662 keV gamma rays [Syntfeld et al. 2005]. LiI:Eu has a
refraction index of 1.96, which gives a critical angle of 49.93◦ at an interface with common glass.
It is notable that in recent work LiI crystals doped with 0.5% Tl yielded 14, 000 ± 1, 400 photons per
MeV [Khan et al. 2015]. Two decay constants were observed, one at 185 ns yielding 88% of the photons
and a slower decay time at 1.089 μs yielding the remaining 12% of photons. The wavelength at the emission
Sec. 13.2. Inorganic Scintillators 507

maxima (λmax ) was measured to be 470 nm. Energy resolution of LiI:Tl was reported to be 8.5% FWHM
for 662 keV gamma rays.
The lithium constituent of LiI:Eu enables thermal-neutron detection through the 6 Li(n,3 H)4 He reaction.
The natural abundance of 6 Li is 7.59%, yielding an atomic density of 6 Li in natural LiI:Eu of 1.39 × 1021
cm−3 . The resulting thermal macroscopic cross section for the 6 Li(n,3 H)4 He reaction is 1.31 cm−1 with
an absorption length of 0.76 cm. If the Li is replaced with enriched 6 Li, the thermal-neutron absorption
macroscopic cross section can be increased to 17.27 cm−1 , and the absorption length is reduced to 0.58 mm.
Further discussion on LiI as a neutron detector is reserved for Chapter 17 on neutron detectors.

Some Other Alkali-Metal Halide Scintillators Once a scintillator has been developed from an alkali-
metal/halogen salt, the obvious question to ask is, what else is there? Indeed, practically all binary combi-
nations of alkali metals and halogens have been studied to determine if they have practical use as radiation
detecting scintillators (except for those compounds based on francium or astatine). Some of these other
combinations did show promise, but simply did not outperform those materials already described in this
section. Combinations in which both constituent atoms are of low Z are less interesting for gamma-ray
detectors and spectrometers, hence can be excluded based on their low interaction efficiency. Described here
are a few of those other possibilities that have relatively high Z elements.
Potassium iodide (KI) was actually investigated by Hofstadter before NaI was, and led to the investigation
of NaI:Tl powders as a scintillator [Hofstadter 1948]. Although relatively bright compared to other known
scintillators at the time, KI:Tl does not have the high light yield produced by NaI:Tl and has a light yield of
approximately only 9,700 photons/MeV [Holl et al. 1988]. It has two main decay branches at 240 ns and 2.5
μs [Robertson and Lynch 1961]. There also appears to be a change in decay constants when irradiated with
alpha particles instead of gamma rays with decay times of 210 ns and 1.76 μs. Milton and Hofstadter [1949]
report λmax = 400 nm with a slightly narrower spread in the emission spectrum than observed with NaI:Tl.
Similarly, Cook and Mahmoud [1954] report λmax = 425 nm; hence, KI:Tl has a similar emission output
as NaI:Tl.15 The index of refraction for KI is 1.68 and has a critical angle of about 63◦ with a common
glass interface. KI has a density of 3.12 g cm−3 , which is lower than that of NaI. Although K is a higher
Z element than Na, it does little to improve the interaction efficiency of KI over NaI because iodine is the
main photon absorber in both materials; hence, the gamma-ray interaction efficiencies are nearly the same.
Along with the problems listed above, natural potassium has a radioactive isotope 40 K, which produces an
intrinsic radiation background with K-based scintillators.
Cesium fluoride (CsF) is a fast inorganic scintillator initially studied by Van Sciver and Hofstadter
[1952]. It has a mass density of 4.12 g cm3 , higher than that of NaI. As with many alkali-metal/halides,
CsF is hygroscopic. CsF scintillates without the assistance of an activator dopant and has λmax = 390
nm [Moszynski et al. 1983]. The absolute photon yield is approximately 1950/MeV at room temperature
[Moszynski et al. 1983; Van Eijk et al. 1993]. CsF has an index of refraction of 1.48, below that of common
glass, so that the critical angle of internal reflection is 90◦ . The measured decay time is 5 ± 1 ns, making it
one of the fastest inorganic scintillators available. These studies revealed that the luminescent efficiency was
much higher for gamma-ray interactions than for alpha particle interactions by approximately a factor of 4
± 10%. It was also observed that the alpha particle pulses were produced by a much slower decay constant
of about 200 ns. These multiple interesting properties make CsF an attractive scintillator for fast timing
applications.

15 KI:Tlhas also been reported to have a broad emission spectrum at room temperature with a λmax of about 301 nm [Edgarton
and Teegarden 1963]. Other measurements indicated λmax of about 410 nm [Smol’skaya et al. 1969] and is similar to that
found by Milton and Hofstadter [1949]. It is quite possible that the samples studied by Edgarton and Teegarden [1963] were
contaminated with additional impurities, yet this possibility is hard to ascertain from the references.
508 Scintillation Detectors and Materials Chap. 13

Cesium Bromide (CsBr) is a heavy element alkali-metal/halide with some interesting properties. It has a
density of 4.44 g cm−3 with an refractive index of 1.7. It is also hygroscopic like many alkali-metal/halides.
CsBr activated with Tl has been reported to have several decay times [Robertson and Lynch 1961; Robertson
et al. 1961]. It was found that CsBr:Tl had two main decay times, which differ with the type of radiation
particle. Notably, alpha particles (5.3 MeV) were observed to produce shorter decay times at 2.3±0.15 μs and
14.5 ± 1.34 μs than electrons (from 662 keV gamma rays) at 2.57 ± 0.13 μs and 24.23 ± 1.5 μs [Robertson and
Lynch 1961]. Pure CsBr also scintillates, although the luminescent yield is poor, reportedly 20 photons/MeV
[Van Eijk et al. 1993]. The decay constant of pure CsBr is unusually short for an alkali-metal/halide at 0.07
ns with λmax = 250 nm.
Rubidium iodide (RbI) has a density of 3.11 g cm−3 with a refractive index of 1.64. It has been reported
to have two decay constants at 1 μs and 200 μs [Birks 1964]. RbI:Tl has a reported emission wavelength of
4.43 nm (at 80 K) [Babin et al. 1999; Zazubovich 2001], with the interesting property that light emission
increases, and the appearance of a luminescent recombination peak of similar intensity appears at 318 nm
when the crystal is placed under stress. Ultimately, the light yield is much lower than that observed for
NaI:Tl. Pure RbI has a third decay constant reported to be 100 μs at low temperature (about 175 K) [Birks
1964]. Natural rubidium has a radioactive isotope 87 Rb, which produces an intrinsic radiation background
with Rb-based scintillators.
Alkali-Earth Halide Scintillators
Alkali-earth halides generally consist of those scintillators possessing the form AB2 , where A is an alkali
earth and B is a halide. These scintillators are usually hygroscopic and are often relatively soft. Many
possess good properties for scintillator detectors, some with good properties for special applications.
Barium Fluoride (BaF2) Barium fluoride is a commercially available scintillator that is slightly hygroscopic.
It is relatively soft with a ranking of 3 on the Moh hardness scale. The mass density of BaF2 is 4.88 g cm−3 ,
and the atomic numbers of the elemental constituents are 56 and 9. The primary interaction efficiency
as a function of gamma-ray energy and detector thickness is shown in Fig. 13.15. It has two important
luminescent emissions at 310 nm and 220 nm,
both intrinsic emissions. The 310 nm lumines-
cent emission has a decay constant τ of 630 ns,
while the 220 luminescent emission has a much
faster decay constant ranging between 600 to
800 ps. The refractive index of BaF2 at 220 nm
is 1.54 and at 310 nm it is 1.50, both practically
the same as common glass windows on PMTs.
Pure BaF2 was initially studied by Faruhki and
Swinehart in 1971, although there was no report
of the short wavelength component at the time.
The absorption of light in common soda-lime
glass is much too high to allow the transmission
of either of the two luminescent wavelengths.
Although some borosilicate glasses can be used
for the 310 nm emissions, they are inadequate
Figure 13.15. The calculated interaction efficiency for photons in
for transmittance of the 220 nm emissions. Per-
BaF2 as a function of energy and detector depth. The probability of haps it is for this reason that the fast lumines-
an initial interaction is shown and not the probability of subsequent cent component remained unreported until 1983
or multiple interactions. [Laval et al. 1983]. Instead, a PMT with a fused
quartz window is preferred if the 220 nm wavelength is to be used (see Chapter 14 on PMTs). Light yield for
Sec. 13.2. Inorganic Scintillators 509

the slow component (310 nm) is about 10,000 photons/MeV and for the fast component (220 nm) is about
1,800 photons/MeV.
As pointed out by Ishii and Kobayashi [1991], BaF2 is mainly important for its fast decay time at the
220 nm emission, and radiation damage that reduces this transmission is of primary concern. Studies by
Messner and Smakula [1960] and also Heath and Sacher [1966] predicted high radiation hardness for BaF2 .
Measurements by Majewski and Anderson [1985] apparently confirm this prediction as fact. They irradiated
BaF2 with energetic protons, with exposures up to 1.3 × 107 rad, and found a loss of only 1%/cm light
transmission. BaF2 crystals have shown good resistance to gamma-ray irradiation up to 106 rad [Woody
et al. 1989]. Another study showed that Pb contaminants in BaF2 significantly reduced radiation hardness
[Murashita et al. 1986]. Is was concluded by Ishii and Kobayashi [1991] that highly purified BaF2 should yield
excellent radiation hardened scintillators. BaF2 did not recover from radiation damage at room temperature
in the study performed by Zhu [1994], although there was indication of partial recovery at room temperature
in the study performed by [Caffrey et al. 1986], or some damage recovery when exposed to sunlight [Murakami
et al. 1991].
An interesting physical aspect to the light emissions from BaF2 is that the 310 nm emission is greatly
affected by temperature changes while the 220 nm emission is not. Studies performed by Schotanus et al.
[1985] revealed that the 310 emission spectrum increases in intensity to approximately 3 times that of its
room temperature output when the temperature is reduced to about 175 K, and practically disappears when
the temperature is increased up to 358 K. However, the 220 nm emission is unaffected by these temperature
changes.
Calcium Fluoride (CaF2 :Eu) Europium doped calcium fluoride, initially reported by Menefee et al. in 1966,
is a commercially available scintillator that is not hygroscopic and is practically insoluble in water. It has
a ranking of 4 on the Moh hardness scale. Because it is not hygroscopic and relatively robust, it can be
used under rough circumstances which would be inappropriate for delicate hygroscopic scintillation crystals.
The mass density of CaF2 :Eu is 3.18 g cm−3 ,
and the atomic numbers of the elemental con-
 
stituents are 20 and 9, both relatively low

for gamma-ray detection. With a photoelec-  !
  

#!


tric/Compton crossover near 70 keV, CaF2 :Eu


 "#!
is best applied for detection of only low energy
gamma rays as can be seen from Fig. 13.16.  $
  
However, CaF2 ;Eu can be used as a beta parti-
 !
 
cle detector because backscattering is reduced "#!
$
#!
by the low Z constituents [Colmenares et al.   
  
1974]. Its primary emission wavelength λmax
$
is 435 nm with a relatively long primary decay 
 $
constant τ of 940 ns. The absolute light yield is
reported to be 19,000 photons/MeV [Saint Gob- 
   

 

ain 2016], approximately 50% of the light yield   
of NaI:Tl. The refractive index at λmax is 1.47, Figure 13.16. Gamma-ray linear attenuation coefficients for a
lower than common glass, indicating that inter- few common scintillators as compared to NaI. Data are from [NIST
nal reflection when coupled to the glass window XCOM].
of a PMT can be minimized to small values.
Calcium Iodide (CaI2 , CaI2 :Tl, CaI2 :Eu) Calcium iodide (doped) is a hygroscopic rare-earth/halogen
scintillator initially studied by Van Sciver and Hofstadter [1951] and Hofstadter et al. [1964a; 1964b; 1967].
Having a similar performance to that of NaI:Tl, this scintillator showed great promise. The pure form of
510 Scintillation Detectors and Materials Chap. 13

CaI2 , along with CaI2 activated with either Tl or Eu, were reported as bright scintillators [Hofstadter et al.
1964b]. The mass density of CaI2 is 3.96 g cm−3 . The initial work on CaI2 was conducted with Tl as the
activator [Van Sciver and Hofstadter 1951]. It was found that CaI2 :Tl had a measured decay constant of
1.1 μs and a light yield approximately the same as that for NaI:Tl. The most probable emission wavelength
(λmax ) was 420 nm. Years later, pure and Eu-activated CaI2 were studied by Hofstadter et al. [1964a; 1964b]
and yielded better results than CaI2 :Tl. It was reported that both pure CaI2 and CaI2 :Eu yielded up to
200% light yield as that for typical NaI:Tl crystals. The most probable emission wavelength for pure CaI2
was 410 nm with a decay constant of 550 ns, and the most probable emission wavelength for CaI2 :Eu was
470 nm with a decay constant of 790 ns [Hofstadter et al. 1964b]. Energy conversion efficiency was calculated
to be approximately 25%. In that same study, energy resolution of 5.19% FWHM was reported for 662 keV
gamma-rays for a CaI2 :Eu sample. Recent work on CaI2 indicates that the theoretically achievable light
yield for CaI2 :Eu is 114,000 photons/MeV, while the measured value was 110,000 photons/MeV [Cherepy et
al. 2009]. Hofstadter et al. [1964b] describe multiple problems with the production of CaI2 crystals, mainly,
the material is more hygroscopic than NaI:Tl and it is also quite easily fractured. CaI2 has a rhombohedral
crystalline lattice formed in a layered structure with weak bonds between the basal planes. Unfortunately,
the crystal is prone to cracking and plastic deformation during both crystal growth and detector fabrication,
and is most likely the reason why CaI2 has not been extensively explored. Methods to improve crystal growth
and material quality have been implemented [Boatner et al. 2015], although the scintillation performance of
these newer high-quality crystals was significantly below that of the earlier results reported by Hofstadter.

Strontium Iodide (SrI2 , SrI2 :Eu) Strontium iodide doped with Eu is a hygroscopic rare-earth/halogen
scintillator, initially studied by Hofstadter [1968], but it received little attention at the time. Recently this
important scintillator has regained attention as a potential high-resolution scintillator. The measured light
yield of 115,000 photons/MeV [Cherepy et al. 2009] is much higher than that of commercially available NaI:Tl
and LaBr3 :Ce scintillators. The most probable emission λmax for Eu-doped SrI2 is 435 nm [Cherepy et al.
2009], and there is a reported broad emission peak that appears between 550 and 600 nm, depending on the
scintillator temperature [Alekhin et al. 2011]. The density of SrI2 (4.55 g cm−3 ) combined with the relatively
high Z constituent atoms (38/53) makes it an efficient gamma-ray absorber. Strontium iodide has a relatively
long decay time of 1.2 μs, a common consequence associated with Eu activators. Unfortunately, the long
decay constant makes SrI2 :Eu less attractive than NaI:Tl and LaBr3 :Ce for many radiation measurement
applications, especially for those with high count rates. The relative light yield is good with a nominally
proportional response down to 15 keV (see Fig. 13.5). It has a refractive index of 2.05 at λmax and a
critical angle with common glass of 47◦ . Energy resolution on the order of 2.7% has been reported for
SrI2 :Eu crystals irradiated with 662 keV gamma rays [Cherepy et al. 2009; Cherepy et al. 2013]. The relative
light yield increases at low temperature (80 K) and decreases significantly at temperatures above 300 K
[Alekhin et al. 2011]. Alekhin et al. [2011] report spectral broadening of the emission spectrum from SrI2 :Eu
as the temperature is increased from 100 K to 600 K. Also reported is an increase in decay constant τ
with temperature going from 400 ns below 100 K to 7 μs at 600 K [Alekhin et al. 2011]. This unusual
increase in τ with temperature is hypothesized to be a consequence of photon self-absorption of emissions
from Eu luminescent centers. Pure SrI2 also scintillates (λmax is about 600 nm), but apparently lacks the
property of an increasing decay constant with increasing temperature; rather there is a decrease in τ at higher
temperatures, ranging from 1.5 μs at 78 K down to 450 ns at 300 K. Recent studies indicate that scintillations
from pure SrI2 are defect (or impurity) related, in that defect-free high purity crystals of undoped SrI2 and
SrI2 :Eu crystals lack this emission altogether [Kawai at al. 2016].
Sec. 13.2. Inorganic Scintillators 511

Transition Metal Scintillators


Yttrium Aluminum Perovskite (YAlO3 :Ce or YAP) Yttrium Aluminum Oxide (or YAP) is a transition
element rare earth (Y) having the general chemical formula of ABO3 , making a mineral of the perovskite16
family. Perhaps the most interesting property of YAlO3 :Ce (YAP:Ce) is its unusually good linearity in the
low energy range, leading to energy resolution approaching the theoretical maximum. With an average light
yield of about 18,000 photons/MeV, is has about 42% of the NaI:Tl light yield, yet the light yield linearity
property of YAP:Ce also produces much better energy resolution. For example, a FWHM energy resolution of
less than 4.4% has been reported for 137 Cs 662 keV gamma rays [Kapusta et al. 1999, Moszynski 2003]. Other
advantages of YAP:Ce include a fast decay time of 27 ns, a relatively high mechanical strength and chemical
stability, and thermal stability [Leroq et al. 2006]. The fast decay time enables fast timing applications, while
the mechanical and chemical robustness reduces problems with detector fabrication (slicing and polishing).
The thermal stability produces a minimal change in performance with temperature variations and allows its
use at higher temperatures than other scintillators. However, disadvantages include relatively low Z numbers
for the constituent elements (39,13,8), a high index of refraction (1.95), and a relatively low value for λmax
of 370 nm. Although the density of YAP is 5.35 g cm−3 (higher than that of NaI:Tl), the low Z elements
yield a relatively low attenuation coefficient at moderate and high gamma-ray energies. The high index of
refraction causes the critical angle for internal reflection at a glass interface to be high, approximately 50◦ .
The low value of λmax causes inefficient coupling to standard bialkali and multialkali PMTs.

Lutetium Aluminum Perovskite (LuAlO3 :Ce or LuAP) Lutetium Aluminum Oxide (LuAP), also a rare
earth perovskite, has many similar properties to YAP. Perhaps the most important differences are LuAP’s
higher density of 8.34 g cm−3 and its higher Z constituent element Lu (Z = 71), both of which significantly
increase its gamma-ray absorption coefficient. It certainly has one of the highest average gamma-ray atten-
uation coefficients of the known scintillators. It is also a fast decay scintillator, with two decay constants
of 16.5 ns and 74 ns. However, the light yield of LuAP is only 11,400 photons/MeV with λmax = 365 nm.
Its index of refraction is 1.94; hence, the critical angle is also approximately 50◦ with most common glasses
used for PMT windows. Consequently, these multiple disadvantages produce a measured energy resolution
usually inferior to that observed with YAP:Ce, although there is at least one report indicating that relatively
good energy resolution can be achieved, namely 6.8% FWHM at 662 keV for small crystals [Balcerzyk et
al. 2005]. Although the light yield is only 26.5% of that of NaI:Tl, its energy resolution can be comparable,
most likely a beneficial consequence of LuAP:Ce having a proportional relative light yield in the low energy
region similar to that observed with YAP [Balcerzyk et al. 2005].

Yttrium Aluminum Garnet (Y3 Al5 O12 :Ce or YAG:Ce) Yttrium aluminum garnet17 YAG:Ce is a non-
hygroscopic relatively fast inorganic scintillator that has found use with scanning electron microscope (SEM)
systems [Autrata et al. 1978; Bok and Schauer, 2014]. It has relatively high resistance to radiation damage,
making it suitable for use under the expected high electron bombardment in a SEM. YAG has a density of
4.55 g cm−3 , and its highest Z component is yttrium (39) so that it has only modest gamma-ray absorption
coefficients. YAG has a cubic crystal structure and rates 8.5 on the Moh hardness scale.
It is yellow in appearance, with a most probable wavelength of emission λmax at 550 nm. Manufacturers
recommend the use of an extended red PMT response, such as the S-20 PMT. However, the use of a silicon
photodiode (Si PD) is a good alternative, mainly because the quantum efficiency is well matched between
a Si PD and the emission spectrum from YAG:Ce. It has an index of refraction of 1.82 that produces a
critical angle of 55.5◦ at a glass interface. Depending on the doping concentration and type of radiation,

16 Discovered in the Ural Mountains in 1839 by Gustov Rose, this mineral is named after the Russian mineralogist Lev Perovski.
17 The word “garnet” is derived from the Middle English word ‘gernet’, which means ‘dark red’.
512 Scintillation Detectors and Materials Chap. 13

YAG:Ce has multiple decay times [Moszynski et al. 1994]. Moszynski et al. [1994] report decay times of
88 ns and 302 ns when irradiated with gamma rays, and decay times of 68 ns and 247 ns when irradiated
with alpha particles. These differences in decay times for heavy charged particles and gamma rays have
been used to discriminate radiation types through pulse shape discrimination [Ludziejewski et al. 1997]. The
absolute light yield is approximately 15,000 photons/MeV if measured with a Si PD, but somewhat less at
1,270 photons/MeV when measured with a PMT [Ludziejewski et al. 1997]. Energy resolution of 11.1% was
reported for 662 keV gamma rays when coupled to a PMT [Moszynski et al. 1994].
Lutetium Aluminum Garnet (Lu3 Al5 O12 :Ce or LuAG:Ce) Closely associated with YAG is LuAG, which
is interesting for gamma-ray detection because of the higher Z component lutetium (71). A comprehensive
review by Nikl et al. [2013] provides general information on its development. LuAG has a crystalline cubic
structure, a density of 6.76 g cm−3 , and rates 8.5 on the Moh hardness scale. LuAG has been discovered to
yield good performance with Ce [Chewpraditkul et al. 2009] and Pr activator dopants [Yanagida et al. 2011].
LuAG:Ce, also yellow in color, has a peak emission wavelength λmax between 510 and 535 nm and a decay
constant between 55 and 70 ns. The absolute light yield ranges between 18,000 and 26,000 photons/MeV and
is relatively proportional above 100 keV [Nikl et al. 2013]. Gamma-ray performance is good, with a reported
FWHM energy resolution between 5.5 and 7% at 662 keV [Nikl et al. 2013 and references therein]. LuAG:Pr
has a reported peak emission wavelength λmax of 310 nm [Świderski et al. 2009a] and a decay constant of
20 ns [Furukawa 2016]. A reported absolute light yield is 22,000 photons/MeV for commercial material
[Furukawa 2016]. The light yield proportionality is quite excellent for energies above 100 keV [Świderski et
al. 2009a], and most likely assists with the good energy resolution observed, with a best resolution reported
as 4.2% at 662 keV for commercial LuAG:Pr [Furukawa 2016].
Zinc Sulfide (ZnS:Ag) Zinc sulfide is a relatively old scintillator, having been discovered by Théodore Sidot
in 1866. It is a non-hygroscopic material with a density of 4.09 g cm−3 . Because of its low Z constituents, it
is not an efficient gamma-ray detector, but is a relatively bright scintillator for heavy charged particles. ZnS
was used as the scintillator for alpha particle counting by Rutherford and Geiger and is also the scintillating
component in common spinthariscopes. There are two main crystalline forms of ZnS that can exist at room
temperature, a cubic (zinc blend) form and a hexagonal (wurtzite) form, which unfortunately makes single
crystal growth difficult and leads to polymorphism. Because of the difficulty in producing single crystals,
ZnS is available either as a polycrystalline powder or as thin optical crystals. ZnS is also a wide band-gap
semiconductor material with the hexagonal and cubic forms having band gaps of 3.91 eV and 3.54 eV,
respectively.
When doped with Ag as an activator, ZnS:Ag has a most probable emission wavelength λmax = 450 nm.
Its refractive index is high at 2.36 that produces a critical angle of 39.5◦ when coupled with glass or acrylic.18
ZnS:Ag has poor light response to gamma rays, but is relatively bright for heavy ion interactions. The light
yield is about 54,000 per MeV for alpha particles, or approximately 126% of the light output of NaI:Tl and
has a reported decay constant of 110 ns [Saint Gobain 2016]. ZnS:Ag in the form of polycrystalline powder
is opaque to its own light emissions for mass thicknesses greater than 25 mg cm−2 (or 61 microns). Hence,
most detectors utilizing ZnS:Ag are limited to thin films. ZnS:Ag is generally used for heavy ion detection.
Two interesting configurations are the Lucas cell and the Hornyak detector.
A Lucas cell is a cylindrical cup configured as a gas-flow chamber, usually with dimensions on the order
of 5 cm in diameter and 5 cm long. The gas-flow chamber has inlet and outlet ports, and the inside of
the chamber is coated with a scintillator, usually ZnS:Ag [Lucas, 1957]. A Lucas cell is designed to accept
a gas sample, filter out the radioactive particulates, and subsequently count radioactive decay products as
they produce scintillation light when they strike the chamber walls. A PMT attached to the open top of

18 Poly(methyl methacrylate) or PMMA, also known as plexiglass or lucite.


Sec. 13.2. Inorganic Scintillators 513

the chamber registers light pulses, thereby producing a count rate from the chamber. A Lucas cell is often
used to measure radon gas concentrations [Abbady et al., 2004]. Radon, a radioactive gas, decays by α
particle emission, which produces a chain of radiative daughter products. Inhalation of radon can result in
radioactive daughter products becoming lodged on the surfaces of the respiratory system, and presents a
health risk in regions of high radon accumulation. The standard for measuring radon gas can be found in
the ANSI/AARST MS-PC 2015 report.
A Hornyak detector [Hornyak 1952], often called a Hornyak button, is a detector configuration used
for fast-neutron detection while suppressing signals from slow neutrons and gamma rays. The original
devices were composed of ZnS:Ag particles interspersed within an acrylic medium. Modern Hornyak buttons
have interspersed concentric cylinders, similar to a “bull’s eye” target, alternating between non-scintillating
acrylic light waveguides and layers of ZnS:Ag. Fast neutrons interact in the plastic and eject protons into
the ZnS:Ag. The energetic protons fluoresce the ZnS:Ag, and a fraction of the light propagates through the
plastic to a light detection device, such as a PMT. Hornyak buttons are used for fast neutron detection in
high gamma-ray environments in order to reduce the background emissions. More detail on this type of
detector can be found in Chapter 18.
Post-Transition Metal Scintillators
Bismuth Germanate (Bi4 Ge3 O12 or BGO) Bismuth germanate, commonly referred to as BGO, is a rel-
atively rugged fracture resistant non-hygroscopic material, and it is rated as 5 on the Moh hardness scale.
BGO has one high Z constituent (Bi = 83, Ge = 32, O = 8), along with a relatively high density of 7.13 g
cm−3 , making it a good gamma-ray absorber. The primary interaction efficiency as a function of gamma-ray
energy and detector thickness is shown in
Fig. 13.17. Ishii and Kobayashi [1991] report
that it is a relatively radiation hard material, ca-
pable of withstanding gamma-ray dose between
104 and 105 rad before showing significant light
absorbance. Because of its high gamma-ray
absorption efficiency, thereby reducing patient
dose, it has found practical use in the medical
imaging industry [Cho and Farukhi 1977]. The
most probable emission wavelength λmax is 480
nm with a decay time of 300 ns. The abso-
lute light yield at room temperature is approx-
imately 8,200 photons/MeV, with a PMT re-
sponse of only 13% relative to NaI:Tl; hence the
gamma-ray energy resolution is poor by compar-
ison to NaI:Tl. BGO also has a lower luminosity
fast emission, yielding about 700 photons/MeV Figure 13.17. The calculated interaction efficiency for photons in
with τ = 60 ns. With a relatively large refrac- BGO as a function of energy and detector depth. The probability of
tive index of 2.15, it has a narrow critical angle an initial interaction is shown and not the probability of subsequent
or multiple interactions.
of 44.2◦ at the glass interface of a PMT window,
making light collection more difficult than with other inorganic compounds with lower indices of refraction.
Overall, energy resolution of 15% FWHM is typical for 662 keV gamma rays [Nestor and Huang, 1975].
BGO scintillates without an activator, the luminescence caused by intrinsic 3 p1 → 1 s0 transitions of the
Bi ions in the crystals [Weber and Monchamp 1973]. The Bi3+ ion actually has a small band gap (about
3+

2 meV) between the excited states 3 p1 and 3 p0 and, thus, has two different transitions, namely the 3 p1 →
1
s0 and the 3 p0 → 1 s0 [Rodnyi 1997]. These two possible transitions help explain the appearance of two
514 Scintillation Detectors and Materials Chap. 13

emission wavelengths and decay times. The Stokes shift is large enough such that BGO is transparent to its
luminescent photons. BGO light yield is significantly dependent upon temperature and shows high thermal
quenching above room temperature. Provided that an adequately long electronic shaping time is applied,
the absolute light yield of BGO at 77 K can be double its room temperature yield (see Fig. 13.8). Ivanov et
al. [1987] report an increase of relative quantum efficiency, compared to NaI:Tl, of 0.13 at room temperature,
increasing to 0.44 at 80 K.

Lanthanide Scintillators
Lanthanide halides are those scintillators with
the chemical makeup of AB3 , where A is an
 
element in the lanthanide series and B is a   
halide. These scintillators are generally very
  


hygroscopic and fragile, but many possess out- 


standing absolute light yield, good relative light
yield proportionality, fast decay times, good 
"#$%
gamma-ray absorption efficiency (Fig. 13.18), 
!
and ultimately superior energy resolution com-

pared to NaI:Tl. Several are now commercially "#$%     
  
 
available, although mainly in sizes of 3 × 3 in   
right cylinders or smaller. For scintillators with
 !
the element La as a main constituent, a defi- 

ciency is the presence of 138 La, which is radioac-


tive with a natural abundance of 0.09%. It emits 
   
low energy beta particles along with 1435.8 keV   
(BR = 0.7) and 788.7 keV (BR = 0.3) gamma
rays. Although the gamma-ray emissions can be Figure 13.18. Gamma-ray linear attenuation coefficients for a few
lanthanide scintillators as compared to NaI. Data are from [NIST
used as intrinsic calibration energies, they un- XCOM].
fortunately also produce an intrinsic radiation
background.

Cerium Bromide (CeBr3 ) Cerium bromide is a lanthanide halide scintillator that has received much atten-
tion in recent years. Although it was synthesized as early as 1899 [Muthman and Stüzel 1899], only recently
was it recognized as a bright luminescent radiation detection material [Shah et al. 2005]. CeBr3 has a density
of 5.1 g cm−3 , and with constituent elements Ce (Z = 58) and Br (Z = 35) it has good gamma-ray absorp-
tion efficiency. CeBr3 has a hexagonal crystal structure, is hygroscopic and fragile, easily cleaving along the
slip planes [Doty et al. 2007]. The most probable light emission is at 390 nm with a decay constant of 19 ns.
The reported light yield is approximately 68,000 photons per MeV [Shah et al. 2005], and the relative light
yield is reasonably proportional above 100 keV, although less so than LaBr3 :Ce for energies below 100 keV
[Khodyuk and Derenbos 2012, Quarati et al. 2013]. Luminescence from CeBr3 arises from an excited state of
the Ce3+ , and it does not require an activator dopant. It has a refractive index of 2.09 at λmax with a critical
angle of 45.9◦ at a common glass interface and with such a high refractive index, significant amounts of light
can be lost from internal reflections. Regardless, energy resolution of 3.2% FWHM at 662 keV was reported
for CeBr3 doped with Ca2+ [Guss et al. 2014]. Methods have been implemented to address the fragility of
CeBr3 , and other lanthanide halides, using aliovalent doping to inhibit cracking and had some promising
success [Harrison et al. 2009]. Tests with gamma-ray irradiation indicate that CeBr3 can withstand dose
exceeding 100 kGy with only a minor decrease is energy resolution performance [Drozdowski et al. 2008b].
Sec. 13.2. Inorganic Scintillators 515

Lanthanum Chloride (LaCl3 :Ce) Cerium activated lanthanum chloride (LaCl3 :Ce) was reported by van
Loef et al. in 2001 as a new bright scintillator that can perform in a fashion similar to that of NaI:Tl. The
combination of a low mass density of 3.84 g cm−3 and only one substantial Z number atomic constituent
La (57) yields LaCl3 :Ce gamma-ray detection efficiency similar to that of NaI:Tl. The material is very
hygroscopic and brittle, and has a hexagonal crystal structure that cleaves easily along the {100} planes.19
The most probable emission wavelength for LaCl3 :Ce λmax is 350 nm, which unfortunately is not well matched
to common PMTs and results in a loss in sensitivity to the light emissions. The refractive index is 1.9, which
produces a critical angle of 52.1◦ with a glass interface. The absolute light yield is 49,000 photons/MeV,
which is higher than NaI:Tl, but because of the spectral mismatch, its photoelectron response with a bi-alkali
PMT ranges between 70% to 90% of that measured with NaI:Tl. Commonly reported energy resolution is
near 4.0% FWHM at 662 keV for various crystal sizes. The good energy resolution observed from LaCl3 :Ce
is most likely due to the relatively good proportionality of the crystal for energies above 30 keV. It is also a
fast scintillator with a decay constant of τ = 28 ns. The light yield from LaCl3 :Ce decreases with decreasing
temperature with an integration time constant of 1 μs; however, if the integration time constant is increased
to 16 μs, the light output response is fairly constant over a wide range of temperatures (see Fig. 13.8).

Lanthanum Bromide (LaBr3 :Ce) Cerium activated Lanthanum bromide (LaBr3 :Ce) was reported in 2002
by van Loef et al. as a new scintillator that can perform with better energy resolution than that of NaI:Tl.
After a lull in the discovery of bright scintillators capable of competing with NaI:Tl performance, the dis-
covery of Ce activated LaBr3 helped reenvigorate the search for bright scintillators. LaBr3 :Ce has a mass
density of 5.06 g cm−3 , and with relatively large
atomic constituents of 57 (La) and 35 (Br),
it has good gamma-ray absorption efficiency.
The primary interaction efficiency as a function
of gamma-ray energy and detector thickness is
shown in Fig. 13.19. The material is very hy-
groscopic and brittle, and has a hexagonal crys-
tal structure that cleaves easily along the {100}
planes.18 The probable emission wavelength for
LaBr3 :Ce λmax is 380 nm, which matches well-
enough with common PMTs. The refractive in-
dex is 1.9 that produces a critical angle of 52.1◦
with a glass interface. The absolute light yield
is 63,000 photons/MeV, and its photoelectron
response with a bi-alkali PMT ranges between
130% to 165% of that measured for NaI:Tl. The
energy resolution achieved is quite excellent for Figure 13.19. The calculated interaction efficiency for photons
a scintillation, with reported values below 2.9% in LaBr3 as a function of energy and detector depth. The proba-
FWHM at 662 keV for various crystal sizes. The bility of an initial interaction is shown and not the probability of
excellent energy resolution is a combined effect subsequent or multiple interactions.
of the absolute light yield and the good relative light yield proportionality. It is also a fast scintillator with
a decay constant of τ = 16 ns, a time which requires that the light detection device be capable of following
such a fast and bright light output without causing space charge buildup.20

19 or, more traditionally, the {101̄0} planes.


20 Charge buildup from dense electron packages in a PMT can alter the internal voltage and produce non-linear output spectra.
516 Scintillation Detectors and Materials Chap. 13

Alternative activator co-dopants have been explored with LaBr3 :Ce scintillators, including Li, Na, Mg,
Ca, Sr, and Ba as co-dopants to Ce [Alekhin et al. 2013a]. Of these, usage of Sr as a co-dopant with Ce shows
excellent improvement, reported as approaching 2% FWHM for 662 keV gamma rays from 137 Cs [Alekhin et
al. 2013b]. This improvement in energy resolution is attributed to a reduction in scintillation light losses from
competing radiationless recombination processes and also an observed increase in light yield. Consequently,
the light response linearity is improved, even in the low energy region between 10 to 100 keV [Alekhin et
al. 2013b]. A drawback to co-doping with Sr is typically longer, and multiple, decay times, including some
phosphoresence with decay times in microseconds.

Rare Earth Orthosilicates


Gadolinium Oxyorthosilicate (Gd2SiO5 :Ce or GSO:Ce) Gadolinium oxyorthosilicate is a lanthanide sili-
cate scintillator discovered in 1982 by Takagi and Fukazawa. It has one element with a high Z constituent
(Gd Z = 64, Si Z = 14, O Z = 8) and also a density of 6.71 g cm−3 and, thus, makes it a relatively efficient
absorber of gamma rays. GSO has a monoclinic crystal structure and is not hygroscopic. Doped with the
activator Ce, it has a fast decay component of 60 ns and a slow decay component of 600 ns. The light yield of
the fast component is about 8,000 photons/MeV with about 20% light response to a common bi-alkali PMT
compared to that of NaI:Tl, and the light yield of the slow component is about 1,000 photons/MeV [Rodnyi
1997]. The most probable decay component is centered at λmax = 430 nm. This emission mechanism is
believed to be mainly from self-trapped holes. GSO has an index of refraction of 1.85 which yields a critical
angle of 54.2◦ at a glass interface and thus indicates that a large percentage of photons can be internally
reflected. Energy resolution of less than 7.0% FWHM at 662 keV has been reported [Melcher et al. 1996,
Kamae et al. 2002]. GSO has a natural radioactive background component from 152 Gd, which has a natural
abundance of 0.2% and emits 2.14 MeV alpha particles.
The migration coefficient of Ce in GSO is near unity, meaning that the dopant is uniform throughout
the crystal [Takagi and Fukazawa 1983]. A uniformity study performed by Ishibashi et al. [1998] indicated
that the GSO doped with 0.5% mol Ce had less than 7% light variation over an ingot 280 mm long and
80 mm in diameter. With growth improvement, excellent results were achieved by Kurashige et al. [2004]
with larger 100-mm diameter and 290 mm long crystals and produced only 0.42% standard deviation in light
yield across the diameter and only 0.4% standard deviation along the length. Further, the decay constant
was shown to be unaffected by small changes in Ce distribution and were found to have less than standard
deviations of 1.7% longitudinally and 1.0% standard deviation radially.
Studies show that GSO is somewhat non-proportional over a wide energy range [Balcerzyk et al. 2000],
but has better proportionality than either LSO or YSO. GSO is also a thermally stable scintillator, and had
been used for oil well logging [Roscoe et al. 1992]. Due to its good gamma-ray detection efficiency and its
superior energy resolution to that of BGO, it has also found some use in medical imaging PET instruments
[Ficke et al. 1994].
The removal of impurities from the crystal improved light yield by a significant amount and increased
the light yield by about 30% [Kamae et al. 2002]. Energy resolution for some of these samples was 6.7%
FWHM at 662 keV. It was also found that co-doping with Zr improved light yield as well and increased the
yield by 20% [Shimura et al. 2006], with best results having a Zr concentration of 200 ppm.
With the enormous thermal-neutron absorption cross section of natural Gd (49,000 b), GSO has been
studied as a possible neutron detector by reliance upon either the prompt reactions 157 Gd(n,γ)158 Gd or
155
Gd(n,γ)156 Gd as the detection mechanism [Reeder 1994]. Conversion electrons and gamma-ray emissions
can be detected after a neutron absorption, and the important characteristic emissions can be absorbed in
only 75 μm of GSO. Unfortunately, GSO is also an efficient gamma-ray detector; hence, it is sensitive to
background radiations that can be falsely interpreted as neutron induced events.
Sec. 13.2. Inorganic Scintillators 517

Lutetium Oxyorthosilicate (Lu2 SiO5 :Ce or LSO:Ce) Cerium activated lutetium oxyorthosilicate (LSO:Ce)
is a relatively new scintillator discovered and developed by Melcher in 1990 [see Melcher 1990; Melcher
1991; Melcher and Schweitzer 1992; Daghighian et al. 1993]. The scintillator was originally developed for
oil well logging measurements, but was found to have severely degraded energy resolution at the elevated
temperatures typically encountered during oil well logging measurements. Further, the energy resolution
was poor compared to common NaI:Tl detectors. However, it was measured to have 75% of the absolute
light yield of NaI:Tl (about 31,000 photons/ MeV), which at the time was a tremendous breakthrough for
inorganic scintillators [Daghighian et al. 1993]. LSO:Ce has a mass density of 7.4 g cm−3 , and with its large
Z number constituent Lu (71), it has excellent gamma-ray absorption efficiency, comparable to that of BGO.
The primary interaction efficiency as a function
of gamma-ray energy and detector thickness is
shown in Fig. 13.20. Daghighian et al. [1993] re-
port two decay constants of 12 ns (30%) and 42
ns (70%), with a most probable emission wave-
length λmax of 420 nm. However, from various
sources, the reported decay constant ranges be-
tween 37 ns to 47 ns [Rexon 2015; Ludziejewski
et al. 1995]. It has relatively proportional light
yield for gamma-ray energies greater than 200
keV, but not below 100 keV. The index of re-
fraction is 1.82 which produces a critical angle of
55.5◦ at a glass interface. The crystal is robust,
is not hygroscopic, and rates 5.8 on the Moh
hardness scale. LSO:Ce has found good use as
a replacement for BGO in PET scan systems
[Daghighian et al. 1993]. It has 190% of the Figure 13.20. The calculated interaction efficiency for photons in
absolute light yield measured for common BGO LSO as a function of energy and detector depth. The probability of
crystals while having almost the same gamma- an initial interaction is shown and not the probability of subsequent
ray interaction efficiency. Energy resolution for or multiple interactions.
662 keV gamma rays as low as 10.3% FWHM have been measured, much better than that for BGO. Further,
it is radiation hard, with a reported radiation limit of greater than 106 rads. A significant problem with
LSO:Ce is that it is naturally radioactive because of 176 Lu (2.59% isotopic abundance) which emits beta
particles and gamma rays. This problem is further exacerbated by unintentional doping with other radioac-
tive impurities from the crystal growth source materials. However, for specific applications such as PET
measurements, which uses coincidence counting, this natural background is of less concern. Another problem
is that LSO:Ce has long phosphorescence, which has been measured to last several seconds [Szupryczynski
et al. 2004]. Nassalski et al. [2007] generally concluded the long phosphorescence precludes LSO:Ce from
application in CT systems because of the detector requirements.

Yttrium Oxyorthosilicate (Y2 SiO5 or YSO:Ce) Ce-doped yttrium orthosilicate (YSO:Ce) is a non-
hygroscopic rare-earth oxyorthosilicate. The material has a density of 4.45 g cm−3 . YSO is disadvantaged as
a gamma-ray spectrometer because of its relatively low Z number constituents (the largest is Z = 39 for Y)
and moderate mass density. YSO:Ce has a most probable wavelength λmax of 420 nm and relatively good
energy proportionality above 100 keV [Cutler et al. 2009]. The decay constant τ is about 50 ns. Commercial
YSO:Ce usually has an absolute light yield around 10,000 photons/MeV [Melcher 1996], although a higher
light yield of about 24,000 photons/MeV has been reported for optimized crystals [Balcerzyk 2000, Cutler
2009]. Co-doping with Ce/Ca has been studied with reportedly small effect and produced an absolute light
518 Scintillation Detectors and Materials Chap. 13

yield of 21,200 photons/MeV. The index of refraction is 1.8 to produce a critical angle of 56.4◦ at a glass
interface. The reported energy resolution often is 9.0% to 9.4% FWHM for 662 keV gamma rays, although
energy resolution as low as 7.4% FWHM has been reported [Dahlbom et al. 1997].
Lutetium Yttrium Oxyorthosilicate (Lu1.8Y0.2 SiO5 :Ce or LYSO:Ce) Lutetium yttrium oxyorthosilicate
(LYSO:Ce) has been grown in an attempt to include the main advantages of both LSO and YSO crystals
[Cooke et al. 2000; Pepin et al. 2004; Chen et al. 2007]. LYSO:Ce is a commercially available scintillator with
similar properties as LSO:Ce [Rexon 2015, Omega 2016]. In summary, the density of LYSO is 7.4 g cm−1
with a refractive index of 1.82. The decay constant has been measured to be between 40 and 44 ns with a
most probable emission wavelength between 420 and 428 nm. It has similar radiation hardness (greater than
106 rad) as LSO, but it produces increased afterglow phosphorescence with increased radiation damage. The
light yield is also the same as LSO, at approximately 31,000 photons/MeV. It is robust, non-hygroscopic with
a Moh hardness of 5.8. Energy resolution is similar to that of LSO, near 10% FWHM for 662 keV [Chen et
al. 2007]. Because of the natural abundance of 176 Lu, it also has an intrinsic radioactive background. Cooke
et al. [2000] report lower temperature dependence on light yield than observed with LSO. Further, Cooke
et al. [2000] note that the main advantages to LYSO over LSO are lower production costs, fewer inclusion
defects in the crystals, and easier incorporation of the Ce activator dopant in the crystal lattice.

Elpasolites
Elpasolites21 are a new class of scintillators of the form A2 BRX6 , where A and B are alkali metals, R is a
rare earth, and X is a halogen. They have essentially a double perovskite structure, and many maintain a
cubic structure over a broad range of formations [see Doty et al. 2012]. The possible combinations number in
the thousands, and several have been identified as potentially good scintillators for gamma-ray spectroscopy
and neutron detection [Gundiah et al. 2014; Wei et al. 2014; Doty et al. 2012]. Listed here are only a few
combinations that show promise.
Cesium Lithium Yttrium Chloride (Cs2 LiYCl6 :Ce or CLYC:Ce) The relatively new cesium-based elpasolite
scintillator Cs2 LiYCl6 :Ce, or CLYC:Ce, is a dual-use inorganic scintillator that can detect both gamma rays
and neutrons. It has a density of 3.31 g cm−3 , with its highest Z component being Cs (Z = 55). However,
the actual density of Cs atoms comes to 6.94 × 1021 cm−3 , approximately 66% of the atomic fraction for
CsI, with an effective atomic number Zeff of 44.5 [Lecoq et al. 2006]. CLYC:Ce is hygroscopic and, thus,
must be encapsulated. The refractive index of CLYC is 1.81, which produces a critical angle at a common
glass interface of 56◦ . CLYC:Ce has decay constants at 600 ns and 6 μs both of which are relatively long
for most scintillator applications [Combes et al. 1999]. The luminescent emissions for Ce doped CLYC are
centered at 372 nm and 400 nm, while undoped CLYC has a single emission centered at 305 nm [Combes et
al. 1999]. With a 1 μs shaping time, between 7,000 photons/MeV (no Ce doping) to 10,200 photons/MeV
(3% Ce doping) are observed. With a longer shaping time of 10 μs, between 22,000 photons/MeV (no Ce
doping) to 10,800 photons/MeV (3% Ce doping) are measured. Despite the relatively low light yield and
long decay constants, good energy resolution has been reported for CLYC:Ce, as low as 4.2% FWHM for
662 keV gamma rays [RMD 2016].
The lithium constituent of CLYC:Ce allows neutron detection through the 6 Li(n,3 H)4 He reaction. For
natural Li as a constituent, the atomic density of 6 Li in CLYC is 2.6 × 1020 cm−3 to produce a macroscopic
cross section for the 6 Li(n,3 H)4 He reaction of 0.248 cm−1 , or an absorption length of about 4 cm. If the Li
is replaced with enriched 6 Li, the thermal-neutron absorption macroscopic cross section can be increased to
3.27 cm−1 , and the absorption length is reduced to 3 mm. Unfortunately, CLYC also has competing neutron
absorbers, mainly Cl (σCl = 33.5 b) and Cs (σCs = 28 and 2.6 b), that ultimately limit its neutron detection

21 The etymology comes from the location where these minerals were first found in El Paso County, Colorado, USA.
Sec. 13.2. Inorganic Scintillators 519

efficiency. With six halogen atoms per molecule, the neutrons lost to parasitic absorptions can be significant,
limiting the maximum thermal neutron detection efficiency to approximately 22% for CLYC:Ce loaded with
natural Li and approximately 78% neutron detection efficiency for CLYC:Ce loaded with enriched 6 Li.
There is also a core valence emission, with a decay constant of 2 ns with a yield of 660 photons/MeV (no Ce
doping) to zero photons/MeV (3% Ce doping), produced by the radiative recombination of a valence electron
with a core hole [Bessiere et al. 2005]. This core valence emission appears under gamma-ray irradiation, but
not under alpha particle irradiation. Hence, detection of this emission can be used to distinguish between
gamma-ray and heavy charged particle emissions such as those produced from neutron interactions.

Cesium Lithium Lanthanum Bromide (Cs2 LiLaBr6 :Ce or CLLB:Ce) Also new is the cesium-based elpaso-
lite scintillator Cs2 LiLaBr6 :Ce, or CLLB:Ce, which also has dual use as a gamma-ray and neutron detector.
It has a density of 4.2 g cm−3 and its highest Z components are Cs (Z = 55) and La (Z = 57). The density
of Cs and La atoms comes to 8.51 × 1021 cm−3 , approximately 81% of the atomic density of Cs in CsI.
CLLB:Ce has multiple decay constants at 55 ns and at about 270 ns, and there is no reported core valence
emission for CLLB. The luminescent emissions for Ce doped CLLB:Ce are centered at 390 nm and 420 nm
[Shirwadkar et al. 2011]. With Ce doping, the luminescent yield is between 50,000 photons/MeV and 60,000
photons/MeV [Glodo et al. 2011; Shirwadkar et al. 2011]. This high light output, along with the fact that
the luminescent yield is more proportional than that found with CLYC:Ce, indicates that CLLB:Ce is a
promising new scintillator. Indeed, energy resolution of 3.0% to 2.9% FWHM for 662 keV gamma rays has
been reported [Glodo et al. 2011; Shirwadkar et al. 2011].
As with CLYC:Ce, the lithium constituent of CLLB:Ce enables neutron detection through the
6
Li(n,3 H)4 He reaction. For natural Li as a constituent, the atomic density of 6 Li in CLLB is 2.16 × 1020
cm−3 to produce a macroscopic cross section for the 4 He(n,3 H)4 He reaction of 0.2027 cm−1 , or an absorp-
tion length of 4.93 cm. If the Li is replaced with enriched 6 Li, the thermal neutron absorption macroscopic
cross section can be increased to 2.67 cm−1 and the absorption length is reduced to 3.75 mm.

Other Notable Elpasolites Other bright elpasolite scintillators that show promise include cerium activated
Cs2 NaLaI6 :Ce, Cs2 LiLaCl6 :Ce, Cs2 NaLaBr6 :Ce, and Cs2 LiLaI6 :Ce. These scintillators are relatively propor-
tional, provide good light yield, and have short decay constants on the order of 50 ns [Doty et al. 2012]. Kerisit
et al. [2014] report that elpasolites with Br as the halogen rather than Cl should theoretically have higher light
yields and quote theoretical light yields above 100,000 photons/MeV for Cs2 LiLaBr6 :Ce and Cs2 LiYBr6 :Ce.
Gundiah et al. [2014] report a good light yield of about 46,000 photons/MeV for Cs2 NaLaBr6 :Ce with an
energy resolution of 3.9% FWHM at 662 keV. Two emission maxima were observed at 387 nm and 415 nm,
both adequately matched to a bi-alkali PMT. A recent introduction to the elpasolite family that shows great
promise is Cs2 LiLa(Br6−x Clx ) or CLLBC:Ce, which has good gamma-ray energy resolution (∼ 3% FWHM
at 662 keV) and retains the neutron detection characteristic of CLYC:Ce [Shirwadkar et al. 2012]. The
substitution of Br for Cl works to reduce parasitic neutron losses, while the substitution of La for Y works
to slightly increase parasitic neutron losses.
Rb2 LiYBr6 :Ce, and many others, show bright light output for neutron absorption [Birowosuto et al.
2008]. Rb2 LiYBr6 :Ce produces prompt reaction products from the 6 Li(n,3 H)4 He reaction, producing between
59,000 ± 5,400 to 83,000 ± 8,300 photons per neutron capture, depending on the Ce3+ doping concentration
(between 0.1 and 0.5 %). The light yield for gamma rays varies between 16,500 ± 1,600 to 23,000 ± 2,300
photons/MeV for Ce3+ for concentrations between 0.1$ and 0.5%, respectively. It has at least three main
decay components, reported as 71 ns (31%), 400 ns (53%), and 1400 ns (16%). Energy resolution for 662
keV gamma rays was reported as low as 4.6% FWHM [van Eijk et al. 2005]. The difference in light output
520 Scintillation Detectors and Materials Chap. 13

between gamma-ray interactions, along with good energy resolution, allows pulse height discrimination
between neutron and gamma-ray events.22

Ceramic and Glass Scintillators


Methods of producing fully transparent ceramic scintillators were initially developed by GE Corporation
[Cusano et al. 1980; Dibianca et al. 1985] and ceramic casting offers an alternative method of scintillator
production to that of growing a single crystal. Although each type of scintillator may have unique manufac-
turing processes particular to the material, there are several steps generally applicable to the manufacture
of ceramic scintillators. The materials should be very pure (greater than 99.99%), near 100% phase purity,
a total high specific surface area greater than 5 m2 g−1 , and a median particle size of 3 microns or less
[Greskovich and Duclos 1997]. The general process involves the production and subsequent introduction of
nanoparticles of scintillator material into a vessel for compaction. This unfired material is usually termed
a “green” ceramic. The green ceramic is then mixed with the requisite scintillator host and fluorescent
activator dopants. This mixing is one of the main advantages of the ceramic process because the desired
activator concentration can be maintained in the ceramic far more easily than with the traditional crystal
growth method. The compacted material is heat treated to temperatures of approximately 1,200◦ C in air,
followed by vacuum sintering (at about 10−6 torr) at temperatures up to 2,000◦C. Finally, hot pressing at
pressures up to 29,000 psi in argon and at a temperature of 2,000◦C is used to achieve a maximum density.
The final product is a ceramic billet with grain sizes on the order of 10 microns.
There are multiple advantages to ceramic scintillators, namely they have a high radiation hardness com-
pared to halide single crystals, they have relatively low production costs, they are hard and non-hygroscopic,
they are machinable, they are environmentally robust, and they can be manufactured in large sizes that
might be difficult to produce as single crystals. Among the earliest materials investigated as ceramic scin-
tillators were BaFCl:Eu, LaOBr:Tb, CsI:Tl, CaWO4 , and CdWO4 [Cusano et al. 1980]. Cubic crystal
structure has been identified as a condition for successful production of high light yield ceramic scintillators
[Debianca et al. 1985]. Non-cubic crystals have increased refraction at the grain boundaries that increases
light self-absorption and ultimately decreases light yield. Unfortunately, the crystal grains for the materials
listed in the patent by Cusano et al. [1980] are non-cubic, except for that of CsI:Tl which is hygroscopic.
Bixbyite ceramic scintillator structures23 were investigated by Debianca et al. [1985], and include Gd2 O3 ,
Y2 O3 , La2 O3 , Lu2 O3 . Neither Gd2 O3 nor La2 O3 are cubic in form, but are made cubic by incorporating
about 50 mole percent of Y2 O3 into the ceramic. Both Y2 O3 and Lu2 O3 are cubic structured. Lu2 O3 :Eu
has been developed for x-ray imaging [Lempicki et al. 2002] and has reported properties of 9.4 g cm−3 mass
density, a λmax of 610 nm, a light yield of about 60% of that of CsI:Tl, and a long decay time constant τ
of 1.3 ms. The production of (Y,Gd)2 O3 :Eu ceramic scintillators led to their incorporation in CT scanners
[Duclos et al. 2003]. The reported properties of (Y,Gd)2 O3 :Eu are a λmax of 611 nm, a decay constant τ of
960 μs, and an optical attenuation coefficient of 1 cm−1 .
Numerous ceramic scintillators have been investigated and much significant progress has been achieved in
recent years. These ceramics include various garnets, perovskites, bixbyites, and pyrochlores24 [Cherepy et
al. 2008]. Two interesting ceramic scintillators recently developed are Gd1.5 Y1.5 Ga2 Al3 O12 (GYGAG) and
Gd0.3 Lu1.6 Eu0.1 O3 (GLO) [Cherepy et al. 2014, 2015]. Cerium doped gadolinium yttrium gallium aluminum
garnet (GYGAG), (Gd,Y)3 (Ga,Al)5 O12 or GYGAG:Ce, have been under development for many years. The

22 Note that the Q-value for the 6 Li(n,3 H)4 He reaction is 4.7 MeV, giving an upper light yield of about 17,300 photons/MeV
as is similar to that for gamma-ray events. However, it is unlikely that gamma rays with energies approaching 4.78 MeV are
fully absorbed, so discrimination is still possible.
23 Named after Maynard Bixby, who discovered the ore in 1897.
24 The etymology comes from the Greek π υ̃ρ (pyr = fire) and χλωρóς (chloros = green) because pyrochlores often turn green

with a common flame blowpipe analysis.


Sec. 13.2. Inorganic Scintillators 521

material is a robust transparent ceramic with mass density of 5.8 g cm−3 and an absolute light yield of
approximately 50,000 photons/MeV. GYGAG:Ce has at least two decay times, a fast component at 250 ns
and a slow component at 1.7 μs. This unfortunate slower component is thought to be a consequence of
the energy transfer process in the scintillator [Cherepy et al. 2011]. Regardless, energy resolution of 4.5%
FWHM at 662 keV has been reported for a GYGAG:Ce sample coupled to a PMT when operated with a 4
μs shaping time. Better energy resolution is achieved when coupled to a Si photodiode with reported values
of 3% to 3.5% FWHM at 662 keV [Cherepy et al. 2015]. Cerium doped gadolinium lutetium europium oxide
(GLO:Eu) is used for MeV-photon radiography. The material has a high mass density of 9.1 g cm−3 and an
absolute light yield of approximately 55,000 photons/MeV [Cherepy et al. 2015].
Ce-activated glass scintillators were originally developed by Corning Glass Company, as evidenced from
the patents listed in the literature [see Ginther and Schulman 1958]. Of these original scintillation glasses,
it was Ce activated high silica glass that performed best [Ginther and Schulman 1958]. Shortly thereafter,
Voitovetskii et al. [1960a, 1960b] reported different compositions of Li2 O·Si2 O:Ce glass as neutron detecting
scintillators. Ginther [1960] determined that a bright variation of a Li glass scintillator was a mixture of
26% MgO, 13% LiO0.5 , 10% AlO1.5 , 50% SiO2 , and 1% CeO1.5 , which yielded a light yield of 14% of that
of NaI:Tl (nominally 5,000 to 6,000 photons/MeV) and has a most probable emission wavelength of about
390 nm. The Ginther and Schulman study revealed that contaminants in the glass can adversely affect
brightness, especially for alkali earths Ca and Ba contaminants.
Glass scintillators can be machined or formed into various shapes that may not be achievable with common
crystalline solids. Further, glass scintillators are relatively robust and shock resistant, and glass scintilla-
tors have a relatively constant light yield over a wide range of temperatures. These scintillators are used
for a variety of applications, including neutron detection,

oil well logging, and charged-particle detection in ex- #
treme environments. Modern commercial Ce-activated
"
Li glass scintillators can be acquired with different Li ac-
tivator concentrations and enrichments such as natural 
"
Li, 96% enriched 6 Li, and fully depleted of 6 Li. Glass
scintillators with 6 Li can be used for combined neutron
 !

and gamma-ray detection, whereas glass scintillators de- 


#
pleted of 6 Li can be used in mixed radiation fields when
neutron induced counts are undesirable. The resulting "
 

neutron attenuation efficiencies for various commercial 

Li glasses are shown in Fig. 13.21. The decay times gen- "

erally range between 20 to 105 ns, and depend on the Li


concentration and the type of radiation particles inter- 
acting in the scintillator. These scintillators have higher
light yields for irradiation by electrons than by alpha
particles, with an α/β ratio of about 0.23. Glass density 
          
is also a function of Li concentration, ranging from 2.42
−3 −3   
g cm for 24% Li up to 2.64 g cm 7.5% concentration
[Scintacor 2016]. The light yield of these glass scintilla- Figure 13.21. Thermal (2200 m s−1 ) neutron absorp-
tors is reported to be between 20% and 30% of that of tion efficiency for various commercial Li glasses. Proper-
anthracene (or 8.7% to 13% of NaI:Tl), depending on ties are listed in Table 13.2.
the type of glass and Li concentration. The index of refraction varies between 1.55 to 1.58 at the peak
emission wavelength [see Table 13.2, also Applied Scintillation 2016].
Other scintillating glasses have been explored and include boron-based scintillating glass and Li glasses
that have been activated with either Tb or Eu. Boron-based glass scintillators have lower light yields than Li
522 Scintillation Detectors and Materials Chap. 13

Table 13.2. Properties of some commercial Ce activated 6 Li-glass


(natural Li/ 95% enriched 6 Li) .
Glass Designation GS1/GS2 GS10/GS20 KG1/KG2
Density (g cm−3 ) 2.64 2.5 2.42
Isotropic Ratio 2.4% 6.6% 7.5%
Refractive Index 1.58 1.55 1.57
Max Emission λ (nm) 395 395 395
Relative Light Yield* 22% - 34% 20% - 30% 20%
Decay Time (ns) 50 - 70 50 - 70 50 - 70
Available Thickness (mm) 0.1 - 10 0.1 - 10 0.1 - 10
Linear Attenuation Coefficient (cm−1 )† GS1: 0.428 GS10: 1.114 KG1: 1.225
GS2: 5.35 GS20: 14.85 KG2: 16.34

Relative to anthracene.

For 2200 m s−1 neutrons.

glasses, and consequently have less practical application [Bollinger et al. 1962]. Glasses with Tb activators
have higher light yields than Ce activated glasses, up to 50,000 photons/MeV [Pavan et al. 1991], and are
reported to be 2 to 3 times more radiation hard than Ce activated glasses. However, the most probable
wavelength of emission is around 550 nm with long decay times of about 3 to 5 ms. Glasses with Eu as
the dopant were found to have a slightly higher light yield than that of Ce activated glass [Fujimoto et al.
2015], namely about 110% of that of a common GS20 Li glass scintillator. The most probable wavelength
of emission is near 450 nm with a relatively long decay time of 1230 ns [Fujimoto et al. 2015].

13.3 Organic Scintillators


Because the energy bands and corresponding energy levels in inorganic H H H
solids appear as a consequence of a periodic potential, dissociation of
the solid either through melting, decomposition, or solvation usually H C H C C
eliminates the luminescence. Organic scintillator luminescence orig- H H
H
inates from molecular π bonds and, thus, is fundamentally different (a) (b)
from inorganic solids that emit light from luminescent centers such as
defects and impurity dopants in a crystalline lattice. Organic scintil- Figure 13.22. Common depiction of σ
lators depend primarily on the molecular structure of the material for and π bonds. In (a), methane is formed
the scintillation mechanism, and as a result, organic scintillators can by four σ bonds between carbon and
four hydrogen atoms. In (b), ethylene is
emit photons as either solids, liquids, or gases. formed with a σ bond and a π bond be-
Overlapping s and p orbitals can form a strong σ bond, for instance, tween the two carbon atoms, with the
as is the case of methane in which the four electrons in the carbon p remaining four hydrogen atoms forming
orbitals combine with the s orbital electrons of four hydrogen atoms to σ bonds with the carbon atoms.
produce CH4 . As described with fundamental organic chemistry, π states appear from the formation of π
bonds, which occur when two p orbitals overlap in a side-by-side configuration. For instance, the simple
molecule of ethylene (C2 H4 ) is formed with the two carbon atoms sharing electrons in two p orbitals, the
first producing a σ bond and the second forming a parallel π bond, while the remaining electrons form σ
bonds with hydrogen atoms (Fig. 13.22).25 Although a π bond is weaker than a σ bond, together they

25 The graphic depiction in Fig. 13.22b is usually used in organic chemistry to depict a π bond. However, the bond should be
more correctly thought of as a single strong electron bond between the carbon atoms with a weaker associated bonded electron
traveling in the vicinity of the bond.
Sec. 13.3. Organic Scintillators 523

produce a stronger bond than either individually. The π bond is a common building block for many organic
scintillation materials, such as found in benzene rings (Fig. 13.23).
In Fig. 13.24 an energy diagram is shown that is typical of an organic scintillator. An independent
molecule of organic scintillation material can have an electron excited through the π states up from the
ground state into an excited singlet state, of which there are many levels. Hence, electrons in the molecule
can be excited through molecular states rather than atomic states.
There are many vibrational states associated with the ground states, typically denoted by S0x in which
x refers to one of the vibrational sub-states. There are also numerous excited singlet states as well as
excited triplet states associated with the carbon π bonds. Electrons that gain energy rise to one of the
excited vibrational states and generally fall rapidly to the lowest S10 state, which then de-excite through
two possible channels. If the electrons de-excite directly from the S10 state to one of the S0x states, the light
emission is rapid and is referred to as scintillation fluorescence. Decay times for fluorescence are typically only
a few nanoseconds, and fluorescent emission can be easily linked to individual radiation events. However, if
the electrons de-excite by crossing to the triplet states T1x and then fall to one of the S0x states, the light
emission is slow and is referred to as scintillation phosphorescence. This second light producing mechanism is
undesirable because phosphorescent emission is slow and continues to produce afterglow for extended periods
of time and, hence, cannot be directly linked to individual radiation events, especially in high-radiation fields.
Regardless, the main point to notice is that organic scintillators depend on the organic structure, often a
benzene ring structure, and do not need activator dopants for the scintillation mechanism. Hence, they also
do not need to be crystalline or polycrystalline in structure. As a result, organic scintillators can be formed
as solids, liquids, gases, and plastics. Some common organic scintillators are listed in Table 13.3.
Organic scintillators are composed mostly of hydrogen and carbon, both of which are poor absorbers
of gamma rays. They are also notoriously non-linear in light output for heavy ion radiation. However,
they are much more linear in response to electrons and beta particles, and the low atomic numbers for the
constituents tend to make light ion backscattering almost negligible. Hence, organic scintillators are usually
used for beta particle and electron detection.
Another use for hydrogen rich detector materials is fast neutron detection. As discussed in Chapter 4,
and later Chapter 18, energetic neutrons lose more energy by scattering from low A materials than high A
materials. Fast neutrons scatter off of the hydrogen and carbon in the organic scintillator, producing recoil
hydrogen and carbon atoms that then slow down by causing ionization and excitation of other molecules in
the organic scintillator. Because organic scintillators depend on molecular structure for light emission, other
materials can be mixed in the scintillator without destroying the scintillation process. For instance 10 B,
6
LiF, or Gd can be mixed into an organic solution or a plastic to make them more sensitive to neutrons.
Likewise, heavy metal particles, such as Pb, can be mixed into the organic or plastic to make them more
sensitive to gamma rays. There is of course a limit to the amount of absorber material that can be added
because the scintillator transparency reduces with increases in foreign material.
Overall, organic scintillators provide an excellent option when a larger less expensive detector is needed.
Although not well suited for use in gamma-ray spectroscopy, they are quite useful as beta particle and fast
neutron detectors. Moreover, because these detectors are composed of hydrogen, carbon, and oxygen with an
average density of 1.032 g cm−3 , they make near “tissue equivalent” detectors, which is desired for dosimetry
measurements.

13.3.1 Theory of Scintillation for Organic Scintillators


Radiation absorption within an organic scintillator produces energetic electrons, or recoil nuclei, that can
continue to travel through the scintillator and excite more electrons. There are many possible vibrational
and rotational energy levels and, consequently, the ground state (S0 ) and the singlet and triplet states (S1
524 Scintillation Detectors and Materials Chap. 13

H
H
H C
C C

H C C H
C
H
(a) (b) (c)
Figure 13.23. Three representations of a benzene ring. The
shorthand version of (b) or the modern shorthand version (c)
are now in more common usage. It is assumed that the “cor-
ner” carbon atoms of the benzene ring are attached to hydrogen
atoms unless otherwise indicated.

p-states
Ip

singlet states triplet states

S3 S30

S21
S2 S20 T3
inter-system
crossing

S13 T2
S12
S1 S11
S10

T1

S03
S02
S0 S01
S00
fluorescent phosphorescent
emission emission

Figure 13.24. Jablonski diagram of the two basic methods by which an organic
scintillator produces light. π electrons in the organic molecule are excited into
upper vibrational states from a radiation event and rapidly de-excite to the lowest
S10 state. Electrons that then de-excite directly to the S0x states contribute to
scintillation fluorescence. Those electrons that transfer to the triplet states fall
to the T10 state, and gradually de-excite to the S0x states, a process known as
phosphorescence. Straight arrows are radiative transitions, while “squiggly” lines
indicate non-radiative transitions. After Birks [1964].
Table 13.3. Common organic scintillator materials and their properties. The light yield is units of % that of anthracene, which, for comparison, is
about 40% that of NaI:Tl.

Scintillator Light λmax τ Density Refract. H/C Loading Softening Notes


Yield (nm) (ns) (g/cm3 ) Index n Ratio Point (◦ C)

Crystalline

Anthracene 100 447 30 1.28 1.595 0.714 215 β det. and spec.
(E)-Stilbene (or trans-Stilbene) 70 410 3.5 0.97 1.658 0.857 ∼125 α, β and n-spec.
Sec. 13.3. Organic Scintillators

p-Terphenyl (doped) 135 420 3.7 1.23 1.65 0.78 ∼213 doped, n-spec.
Pyrene 60a 477 90 1.27 1.85 0.625 ∼146
p-Quaterphenyl 85a 438 8 0.75 ∼318 difficult to grow
Diphenylacetylene 40a 390 7 0.99 1.606 0.714 62.5
Naphthalene 15 345 75 1.15 1.58 0.8 ∼79 low light yield

Liquid

Legacy Saint- Eljen Rexon


Standardb Gobain

NE 220 BC 220 EJ 351 65 425 3.8 1.036 1.44 1.65


NE 213 BC 501A EJ 301 78 425 3.2 0.87 1.505 1.212 26 γ, fast n
NE 224 BC 505 EJ 305 80 425 2.5 0.877 1.505 1.331 48 γ, fast n
EJ 309 75 424 3.5 0.964 1.57 1.25 144
NE 226 BC 509 EJ 313 20 425 3.1 1.61 1.377 0.0035 F 10
NE 235H BC 517H EJ 321H 52 425 2 0.86 1.48 1.89 81
NE 235L BC 517L EJ 321L 39 425 2 0.86 1.47 2.01 102
BC 517P 28 425 2.2 0.85 2.05 115
BC 517S 66 425 2 0.87 1.70 53
NE 235C BC 519 EJ 325 60 425 4 0.87 1.49 1.73 63
NE 323 BC 521 EJ 331 60 425 4 0.89 1.5 1.31 Gd (1%) 44 n-spec, neutrino
BC 523 65 425 3.7 0.916 1.74 B (5%) -8 n-spec
10
NE 321A BC 523A EJ 339A 65 425 3.7 0.916 1.411 1.67 B (5%) -8 n-spec
BC 525 EJ 335 55 425 3.8 0.88 1.49 1,56 Gd (1%) 91
BC 531 59 425 3.5 0.87 1.63 93
BC 533 51 425 3 0.80 1.96 65
2
NE 230 BC 537 EJ 315 61 425 2.8 0.954 1.498 0.99 D:C H -11
NE 314A BC 551 40 425 2.2 0.902 1.31 Pb (5%) 44
BC 553 34 425 3.8 0.951 1.47 Sn (10%) 42

(cont.)
525
526
Table 13.3. (cont.) Common organic scintillator materials and their properties. The light yield is in units of % that of anthracene, which, for comparison,
is about 40% that of NaI:Tl.

Scintillator Light λmax τ Density Refract. H/C Loading Softening Notes


Yield (nm) (ns) (g/cm3 ) Index n Ratio Point (◦ C)

Plastic

Legacy Saint- Eljen Rexon


Standardb Gobain
NE 102A BC 400 EJ 212 RP 400 65 423 2.4 1.032 1.58 1.103 70 general purpose
EJ 214 59 435 2 1.02 1.58 1.109 60 ultra-thin (250 nm)
NE 104 BC 404 EJ 204 68 408 1.8 1.032 1.58 1.107 70 large area
Pilot F BC 408 EJ 200 RP 408 64 425 2.1 1.032 1.58 1.104 70 general purpose
NE 110 BC 412 EJ 208 60 434 3.3 1.032 1.58 1.104 70
BC 416 RP 200 38 434 4.0 1.032 1.58 1.110 70
Pilot U BC 418 EJ 228 67 391 1.4 1.032 1.58 1.100 70
Pilot U2 BC 420 EJ 230 64 391 1.5 1.032 1.58 1.102 70
NE 111A BC 422 EJ 232 RP 422 55 370 1.6 1.032 1.58 1.102 70 fast timing
BC 422Q 11 370 0.7 1.032 1.58 1.102 C13 H10 O 70
(0.5%)
NE 103 BC 428 EJ 260 36 480 12.5 1.032 1.58 1.103 70
BC 430 45 580 16.8 1.032 1.58 1.108 70
2
BC 436 52 425 2.2 1.032 1.58 0.96 D:C H (13.8%) 70 Thin disks
BC 440 EJ 244 RP 440 60 434 3.3 1.032 1.58 1.104 99
BC 440M 60 434 3.3 1.039 1.58 1.104 100
NE 115 BC 444 EJ 240 RP 444 41 428 285 1.032 1.58 1.109 70 phoswich detectors
BC 448 EJ 248 60 425 2.1 1.032 1.58 1.104 99
NE 142 BC 452 EJ 256 RP 452 32 424 2.1 1.080 1.58 1.134 Pb (5%) 60
BC 454 EJ 254 48 425 2.2 1.026 1.58 1.169 B (5%) 60
NE 105 BC 470 EJ 252 RP 470 46 423 2.4 1.032 1.58 1.037 70 dosimetry
BC 480 *c 425 1.032 1.58 1.100 70
BC 482A EJ 280 *d 494 12.0 1.032 1.58 1.110 70
EJ 284 608 14.0 1.032 1.58 1.110 75
NE 120 BC 490 EJ 290 55 425 2.3 1.032 1.58 1.103 70
BC 498 65 423 2.4 1.032 1.58 1.103 70
EJ 299-33A 56 420 γ13,35,270 1.08 1.58 1.106 n/γ PSD
EJ 299-34 n 13,50,460
a
Adjusted to the S-11 response of a PMT.
b
NE: Nuclear Enterprises, Inc., San Carlos, CA; Pilot: Pilot Chemical Company, Cambridge, MA.
Scintillation Detectors and Materials

c
QE = 0.86.
d
Ratio of Cerenkov light to scintillator light = 10:1.
Chap. 13
Sec. 13.3. Organic Scintillators 527

excited
singlet excited
triplet

ground
(a) (b) (c)

Figure 13.25. Shown are (a) an organic molecule singlet


ground state, showing up and down spin of the electrons, (b)
the singlet excited state, and (c) the triplet excited state. Note
that the electron spins are alike in the triplet state, thereby
through the Pauli exclusion principle, preventing the excited
electron from dropping to the ground state.

and T1 ) have many vibrational states. The energetic electrons are excited from the ground state into many
of these possible vibrational states.
Electron spins are paired in singlet states, and the spin of an excited electron in a singlet state (S10 for
instance) is still paired with the ground state electron. However, electrons in triplet states are no longer
paired to electrons in the ground state, meaning they have identical spin and, therefore, cannot make the
transition because of the Pauli exclusion principle (Fig. 13.25). Note that direct excitation to a triplet state
from the ground state involves a forbidden spin transition and is, thus, improbable.
Electrons can be excited to upper singlet vibrational levels,
which include the various S1 , S2 and S3 levels. The electrons in absorption emission
the higher S1 levels quickly drop to the S10 state within about
10−12 seconds, while electrons in the higher S2 and S3 states
intensity

rapidly relax to the S1 through non-radiative processes. Elec-


trons can also transfer to triplet states by S1 →T1 , a process
referred to as non-radiative intersystem crossing, by which the
spin of electron is reversed. The probability of intersystem cross-
ing increases when the vibrational levels of the two excited states
wavelength
overlap, mainly because little or no energy must be gained or lost
S13
in the transition. Further, intersystem crossing apparently in- S12
creases with molecules with high-Z atoms [Kearvell and Wilkin- S1 S11
S10
son 1968].
The relaxation process for S1 →S0 is a spin-allowed transi-
tion and generally occurs on a times scale of a few nanoseconds.
However, because T1 →S0 is spin-forbidden, the transition takes S03
significantly longer, on the order of μs to ms. This slow process S
S0 S02
of luminescence, thus, gives rise to phosphorescence. 01
S00
As with luminescent centers in inorganic scintillators, there absorption emission
is also a Stokes shift with organic scintillators and can be un-
derstood by reviewing Fig. 13.2. However, now the vibrational Figure 13.26. Depiction of absorption and
states are molecular for organic scintillators. Shown in Fig. 13.26 emission spectra from an organic scintillator.
Adapted from Adachi and Tsutsui [2007].
is a depiction of the origins of the absorption and emission spec-
tra from an organic scintillator. Electrons excited from the ground state (S0 ) up to an excited vibrational
state (S1 states) quickly deexcite to the S10 state through non-radiative processes. Because there are many
possible excited vibrational states, the absorption efficiency is a function of the allowed transitions (see
528 Scintillation Detectors and Materials Chap. 13

Fig. 13.26). These excited electrons can radiatively deexcite to the many possible ground states, which
release photons at wavelengths corresponding to the energy loss between the different states. The lumines-
cent transition from S10 →S00 appears identical to the absorption transition S00 →S10 , but is in fact of lower
energy because of the Stokes shift.
Light Yield
Solid organic scintillators generally produce higher light yields than organic liquids or gases primarily because
of the efficient transfer of energy between luminescent centers. Although organic scintillators should produce
the same luminescent spectrum in either a solid or as independent molecules, significant changes can be
observed because intermolecular complexes that can form between molecules in a solid and because of the
differences in the energy transfer mechanism between molecules [Adachi and Tsutsui 2007]. Impurities in
the organic crystal can also change the luminescent spectrum because efficient energy transfer allows trace
impurities to become the primary luminescent center rather than the host molecule.
Studies performed by Bowen et al. [1949] with mixtures of organic crystals lead to the hypothesis that
energy transfer between organic molecules was substantially due to exciton transfer. This transfer sequence
would progress until the exciton was ultimately captured. Birks and Black [1951] showed that light output
decreased in anthracene when electron irradiation was replaced by alpha particle irradiation. The explanation
for this light reduction is that the damage caused by heavy ions created competing trapping centers, which
could also capture excitons, and as a result caused luminescent quenching. From these observations, a
semi-empirical dependence of light yield as a function of energy deposition was proposed by Birks [1951].
The number of excitons produced in the scintillator per unit path length of travel by the radiation particle
can be described by A(dE/dx) where A is a proportionality constant and dE/dx is the ion energy loss
(or energy deposition) per unit pathlength of travel. Further, the local concentration of ionized molecules,
excited molecules, and damaged molecules along the ion path, can be described by B(dE/dx), where B is
also a proportionality constant. If one defines k as the probability that an exciton is lost to a non-radiative
transition, the specific fluorescence is26

dL A dE/dx
= , (13.36)
dx 1 + kB dE/dx

where the product kB is the quenching parameter. If the energy loss is small, or the corresponding damage
is small, as observed with fast electrons and beta particles, then Eq. (13.36) reduces to

dL dE
≈A , (13.37)
dx dx
which shows a linear relationship with light yield and energy deposition. However, if the energy loss is large,
and the corresponding damage is significant, such as that produced by protons, alpha particles and fission
fragments,
dL A
≈ , (13.38)
dx kB
which implies constant light output regardless of energy deposition. For most organic scintillators, fast
electrons and beta particles with energies above 125 keV do in fact have a relatively linear light yield
response. For slow electrons and beta particles with energies below 125 keV, dE/dx increases and produces

26 Equation (13.36) is often referred to as “Birks’ Equation” or “Birks’ Law”, although John Birks did not promote the name.
Also, B is sometimes referred to as Birks’ constant, although it appears in Eq. (13.36) mainly because the letter ‘B’ conveniently
follows ‘A’ in the English alphabet, and not because it is the first letter in the name ‘Birks’. Birks named the product kB the
‘quenching parameter’ [Birks 1964].
Sec. 13.3. Organic Scintillators 529

(a) (b)

Figure 13.27. (a) Relative scintillation response for different energies of electrons, protons, deuterons, and alpha particles
in anthracene. Data are from Birks [1951]. (b) Variation of specific fluorescence dL/dx with specific energy loss dE/dx for
electrons, protons, and alpha particles in anthracene. Also shown are results from a linear dependence (Eq. (13.38)) and the
dependence expressed by Eq. (13.36) with kB = 6.6 mg cm−2 MeV−1 and kB = 9.3 mg cm−2 MeV−1 . Data are from Brooks
[1956].

a non-linear output in dL/dx. This effect is also apparent for protons, alpha particles and heavy ions. The
severity of the effect in anthracene is shown in Fig. 13.27. In Fig. 13.27(a) there is shown a clear difference
in total light yield as a function of particle type and energy. Shown in Fig. 13.27(b) the dramatic effect of
Eq. (13.37) is apparent where it is seen that as dE/dx becomes large the value of dL/dx becomes constant.
Note that specific energy loss described by the Bragg distribution is highest near the end of the particle
range for protons, deuterons, and alpha particles. Hence, dL/dx tends towards a constant value as these
heavy particles slow down.
A parameter sometimes quoted for organic scintillators is the α/β ratio, which is defined as the ratio of
light produced by 210 Po (5.3 MeV) alpha particles to light produced by 137 Cs conversion/Auger electrons
(624 keV),27
A
α (L/E)|α (dL/dE)|α (dE/dx)|α (dE/dx)|α
=  = kB = . (13.39)
β (L/E)|e− (dL/dE)|e− A kB
The quenching parameter can be approximated for a scintillator by measuring the α/β (or α/e− ) light ratio,
(dL/dE)|e− (dE/dx)|α
kB = = . (13.40)
(dL/dx)|α (α/e− )
Quenching factors have been measured [Czirr 1964] and calculated for a few common organic and inorganic
scintillators by Tretyak [2010] and Nyibule et al. [2014]. There has been work published aimed at refining
the accuracy of Eq. (13.36) by adding more terms to the equation to mainly address the non-linear light
output from heavy ions in organic scintillators [Blanc et al. 1964; Smith et al. 1968; Craun and Smith 1970].
Craun and Smith [1970] propose the addition of a third term,
dL A dE/dx
= . (13.41)
dx 1 + kB dE/dx + C (dE/dx)2

27 In reality, the 624-keV conversion electron is emitted by 137m 137 Cs. The same
56 Ba the daughter produced in the beta decay of
is true for the 662-keV gamma ray commonly attributed to 137 Cs. But the usage here is almost universally used.
530 Scintillation Detectors and Materials Chap. 13

(a) (b)

Figure 13.28. Semiempirical curve fits to luminescent yields from electrons and protons in (a) an-
thracene and (b) (E)-stilbene scintillators. Data are from Smith et al. (1968); curve fitting parameters
are from Craun and Smith (1970).

(a) (b)

Figure 13.29. Semiempirical curve fits to luminescent yields from electrons and protons in (a) NE-
102 (plastic) and (b) NE-213 (liquid) scintillators. Data are from Smith et al. (1968); curve fitting
parameters are from Craun and Smith (1970).
Sec. 13.3. Organic Scintillators 531

Shown in Fig. 13.28 and Fig. 13.29 are comparisons of empirical results from Eq. (13.36) and Eq. (13.41)
for organic crystals of anthracene and trans-stilbene, organic plastic NE-102, and organic liquid NE-213
luminescent light yields. Equation (13.41) with the additional parameter appears to fit the low energy data
better than Eq. (13.36). Quenching parameters kB and C for a few organic scintillators are available in the
literature [Craun and Smith 1970].
Decay Time
A generally accepted description of light emission uses the same theory of Eq. (13.26) (repeated here for
convenience), in which there is a given rise time τr to populate the S10 π states and a given decay time τd
to decay through the S10 → S00 process. The light emission as a function of time is thus given by
Nc (t) N
L(t) = = e−t/τr − e−t/τd .
τd τr − τd
The population rise time τr is usually only a
fraction of a nanosecond, while τd is usually
only a few nanoseconds. However, most organic
scintillators have complex decay schemes that
are difficult to model with a simple exponen-
tial equation. This difficulty is largely due to
changes in decay time with the type of radia-
tion particle and the fact that there often are
multiple decay times involved.
By inspection, the two decay modes seem
to appear, typically labeled fast and slow decay
components. An example is seen from the emis-
sions from trans-stilbene which are shown in
Fig. 13.30. Owen simplified the luminescent de-
cay by assigning only two decay constants to the
light yield of organic scintillators, one fast decay
time τf and one slow decay time τs [Owen 1959].
It is the fast component of an organic scintilla- Figure 13.30. Luminescent decay from (E)-stilbene for alpha parti-
tor that is most often quoted in the literature. cles, neutrons, and gamma rays. Data are from Bollinger and Thomas
[1961].
The short decay times were quite different for
the organic crystals studied and listed in Table 13.3. Owen found that the long decay times were similar for
anthracene, trans-stilbene, and quaterphenyl, ranging between 350 ns and 370 ns. These long decay times
differed with the type of radiation absorbed, showing marked differences between neutron (n, p) events and
gamma-ray events.
Another modification was suggested by Bengsten and Moszynski [1974], who proposed that the rise
time of the pulse be represented by a Gaussian distribution f (t) with σ́ET as the standard deviation. This
additional modification takes into account energy transfer and wavelength shifting in the scintillator along
with time spread in the PMT. Bengsten and Moszynski [1974] successfully apply this modification to specific
plastic scintillators.
Pulse Shape Discrimination
Inspection of Fig. 13.30 reveals major differences among the light emission pulse shapes from alpha particles,
neutrons, and gamma rays. This known phenomenon can thus be used to distinguish among different particle
events in a mixed radiation field [Wright 1956; Owen 1958; Bollinger and Thomas 1961; Brooks and Jones
1974; Yanagida et al. 2015]. Pulse shape discrimination (PSD) can be used to match the decay time of the
532 Scintillation Detectors and Materials Chap. 13

short component to the most probable interacting particle, mainly because the short decay time is strongly
dependent on the type of incident particle. This comparison can be accomplished by plotting the ratio of
light released by the slow component and the fast component (ordinate) against the light released by the
fast component (abscissa), and thus produces a two-dimensional map that separates neutron induced events
from gamma-ray events [Zaitseva et al. 2009; Yanagida et al. 2015].
Another discrimination method is to find the
Dtf Dts ratio of integrated signals (the charge integra-
tion method) produced during separate time pe-
number of events
pulse output

gamma rays threshold riods, Δtf and Δts , that span the decay periods
neutrons of the fast and slow components. A histogram
of events (ordinate) is then plotted against this
neutrons
ratio as in Fig. 13.31(right). The method to pro-
gamma rays duce a useful ratio of fast to slow signal com-
ponents may vary, but ultimately the concept
0 time slow/fast ratio
is the same. Several other methods have been
Figure 13.31. (left) Depiction of scintillation pulse output for explored to produce improved results for PSD
gamma rays and neutrons. (right) Depiction of a histogram of events [Back et al. 2008; Griffiths et al. 2018].
versus the slow/fast integrated signal ratio, which shows a clear dif-
ference between gamma-ray and neutron related events.
Often a clear spectral separation appears, es-
pecially between heavy ions and gamma rays so
that events below a designated slow/fast threshold are attributed to gamma rays and events above the
slow/fast ratio threshold are designated as neutron events. Once this cutoff threshold is determined, modern
electronics can quickly process information in real time to discriminate between neutron and gamma-ray
events. Because organic scintillators can be used as fast neutron detectors from (n, p) reactions, either
method provides a means to discriminate between neutron induced events and gamma-ray induced events
[Yanagida et al. 2015].

13.3.2 Organic Crystalline Scintillators


Although the first scintillators used for radiation detectors were inorganic (ZnS:Ag and PtBa(CN)4 ), it was
naphthalene, an aromatic hydrocarbon crystalline solid, coupled to a photomultiplier tube that was first
used as a practical scintillation detector [Broser and Kallman 1947b; Hofstadter 1975]. Shortly thereafter,
anthracene, an organic compound similar to naphthalene, was shown to be a relatively bright scintillator
[Bell 1948]. Birks [1964] lists numerous organic crystalline solids as scintillators, a few of which are described
here (see also Table 13.4).

Anthracene
Anthracene is one of the brightest organic scintillators available, and has a light yield of about 17,000
photons/MeV, or approximately 43.5% of the light yield of NaI:Tl (see Table 13.3). Anthracene is classified
as an aromatic hydrocarbon. Just as inorganic compound scintillators are traditionally compared to NaI:Tl
for relative performance, the relative brightness of most organic compounds is compared to that of anthracene
whose brightness is taken as 100%. This relative benchmark comparison arises because anthracene is one
of the first bright organic scintillators discovered. However, the relative light yield from anthracene is not
only a function of particle type, but also the particle trajectory within the crystalline lattice [Tsukada and
Kikuchi 1962; Tsukada et al. 1965; Oliver and Knoll 1968], a common trait for crystalline organic scintillators
[Brooks and Jones 1974]. Birks [1964] considered this anisotropic light emission characteristic a fundamental
drawback to having anthracene as the light yield scintillation standard for organic scintillators. The most
probable wavelength of emission is approximately 447 nm, as depicted in the spectrum of Fig. 13.33. The
decay time is approximately 30 ns and is fast compared to most inorganic scintillators. Anthracene can
Sec. 13.3. Organic Scintillators 533

(a) (b)

Figure 13.32. (a) Scintillation decay response in anthracene from gamma rays and neutrons. (b) Histogram of gamma-
ray and neutron events versus the fast/slow integrated signal ratio for Δtf = 20 to 40 ns and Δts = 40 to 150 ns. Data
are from Yanagida et al. [2015].

Figure 13.33. Emission spectrum from crystalline an- Figure 13.34. Absorption and emission spectra from
thracene. Data are from Sangster and Irvine [1956]. anthracene dissolved in cyclohexane and fluoresced
with 235.7 nm light. Data are from Berlman [1971].

be used for pulse shape discrimination between heavy ions, neutrons, and beta particles. Anthracene was
shown in a recent study to be superior for neutron/gamma-ray pulse shape discrimination (PSD) over that
for trans-stilbene and p-terphenyl and showed a clear distinction between neutron and gamma-ray events
Fig. 13.32 [Yanagida et al. 2015].
The mass density of anthracene is 1.25 g cm−3 with a molecular weight of 178.23 g mol−1 . The refractive
index of anthracene is 1.595, closely matching that of common borosilicate glass used for PMT windows.
Anthracene crystals have a monoclinic lattice, and the chemical structure of anthracene (C14 H10 ) is shown
in Table 13.4. The melting point of anthracene is 215.76◦C.
Anthracene can be used in crystalline form, but must be encapsulated to prevent the formation of an
oxidation layer on the outer surface. This surface layer behaves as a quenching region, thereby reducing the
absolute light yield and prolonging decay times. The decomposition of the surface through photo-oxidation is
also promoted by exposure to light if not encapsulated. Anthracene is also fragile and can be easily fractured.
534 Scintillation Detectors and Materials Chap. 13

Table 13.4. Chemical formulas and structures of a few crystalline organic scintillators.

Fluor Chemical Formula Chemical Structure

Naphthalene C10 H8

Anthracene C14 H10

Diphenylacetylene C14 H10

(E)-Stilbene C14 H12

Pyrene C16 H10

p-Terphenyl C18 H14

p-Quaterphenyl C24 H18

Anthracene can be dissolved in a solvent and used as a liquid scintillator, although the emission spectrum
appears to shift (see Fig. 13.34). When dissolved in cyclohexane, the emission peak shifted to 401.6 nm with
a decay time of 4.9 ns [Berlman 1971].

Pyrene
Pyrene is an aromatic hydrocarbon composed of four benzene rings with chemical formula C16 H10 and
monoclinic crystal structure (Table 13.4) [Camerman and Trotter 1965]. The relative light yield of pyrene is
60% that of anthracene and has a most probable emission wavelength of 477 nm [Birks 1964]. The emission
spectrum is shown in Fig. 13.35. The decay time of pyrene is relatively long for an organic scintillator at 90
ns. The mass density of pyrene is 1.27 g cm−3 with a molecular weight of 202.25 g mol−1 . The refractive
index of pyrene is 1.85, which produces a critical angle of 54◦ at a glass interface. The hydrogen to carbon
(H/C) ratio is 0.625. Pyrene begins to soften at 146◦C.

p-Quaterphenyl
One of the many p-oligophenylenes studied as scintillator solutes is p-quaterphenyl which has a molecular
formula C24 H18 (see Table 13.4). The p-oligophenylenes are aromatic hydrocarbon compounds composed
of rings united in the para position by single σ bonds and their general formula is C6n H4n+2 , where n is
the number of rings and n ≥ 3. It has a relatively high light yield of about 85% of that of anthracene
[Birks 1964]. The maximum emission wavelength λmax is 438 nm with a decay constant between 7 and
8 ns. The emission spectrum is shown in Fig. 13.36. The melting point is near 150◦C. Pure crystals of
p-quaterphenyl are difficult to produce and the material is usually available only in powder form and, thus,
may have contributed to its limited use.
Sec. 13.3. Organic Scintillators 535

Figure 13.35. Emission spectrum from crystalline pyrene. Figure 13.36. Emission spectrum from crystalline p-
Data are from Sangster and Irvine [1956]. quaterphenyl. Data are from Sangster and Irvine [1956].

T rans-Stilbene
The organic trans-stilbene (or (E)-stilbene or diphenyl-ethylene) is a diphenylpolyene and is historically one
of the more important crystalline scintillators. It has a mass density of 0.97 g cm−3 , a molecular density of
180.25 g mol−1 , and a chemical formula C14 H12 . The light yield is approximately 70% that of anthracene,
which makes it a relatively bright organic crystal. The
wavelength at maximum (λmax ) is near 400 nm with
a fast decay time of 3.5 ns. The emission spectrum
is shown in Fig. 13.37. The refractive index of trans-
stilbene is 1.62 that produces a critical angle of 67.6◦
at a glass interface. As observed with many other or-
ganic crystalline scintillators, the light yield in trans-
stilbene is directionally dependent upon the interacting
particle trajectory [Hansen and Richter 2002; Cvachovec
et al. 2002]. Stilbene is non-hygroscopic and relatively
non-flammable (NFPA 704 rating of ‘1’), thus making it
relatively easy to process.
It has a melting point of 125◦C and transparent crys-
tals can be grown with the Bridgman technique. How-
ever, these melt-grown crystals are generally limited to Figure 13.37. Emission spectrum from crystalline trans-
small sizes. Recently, large faceted transparent crystals stilbene. Data are from Sangster and Irvine [1956].
of trans-stilbene with 10-cm dimensions have been grown through solution methods [Zaitseva et al. 2011a;
Carman et al. 2013; Zaitseva et al. 2015] and are now commercially available [Inrad 2016]. As a result there
has been renewed interest in trans-stilbene as a fast neutron detector. These solution-grown crystals can be
machined into varying shapes, and reportedly have similar performance as traditional Bridgman-grown crys-
tals [Zaitseva et al. 2015]. Stilbene can be used for pulse shape discrimination between heavy ions, neutrons,
and beta particles [Bollinger et al. 1961; Konobeevski et al. 2012; Yanagida et al. 2015]. The work of Harihar
et al. [1977] indicates that the short decay time of trans-stilbene is mostly unaffected by the magnitude
536 Scintillation Detectors and Materials Chap. 13

(a) (b)

Figure 13.38. (a) Scintillation decay response in trans-stilbene from gamma rays and neutrons. (b) Histogram of
gamma-ray and neutron events versus the fast/slow integrated signal ratio for Δtf = 20 to 40 ns and Δts = 40 to
150 ns. Data are from Yanagida et al. [2015].

of the specific energy loss dE/dx while the long decay time increases with dE/dx. Zaitseva et al. [2011b]
report on the use of trans-stilbene and mixed organic crystals of trans-stilbene for fast neutron detection
using PSD methods. According to the results of Yanagida et al. [2015], shown in Fig. 13.38, trans-stilbene
is a good scintillator for fast neutron PSD, yet not quite as good as anthracene and p-terphenyl. Overall,
trans-stilbene is a good choice for fast neutron detection because it is relatively bright, can now be acquired
in large sizes, is optically clear, fast, and couples well to common PMTs.
p-Terphenyl
Another p-oligophenylene studied as a scintillator solute is p-terphenyl, having molecular for-
mula C16 H14 (see Table 13.4). Pure crystals of p-terphenyl have a light yield of about 40%
compared to that of anthracene [Birks 1964]. However, commercially produced large crystals
of doped p-terphenyl are available with reported light yields that is 135% that of anthracene
[Proteus 2016; Cryos-beta 2016]. The density of p-
terphenyl is 1.23 g cm−3 with molecular weight of 230.
The H/C ratio is 0.778 and the melting point is 213◦ C.
This organic scintillator is relatively fast with decay
times between 3.0 and 3.7 ns. The maximum emis-
sion wavelength λmax is 420 nm, which matches well
to common bi-alkali PMTs. The emission spectrum is
shown in Fig. 13.39. The refractive index is 1.65 with
a critical angle of about 65◦ C at the interface of com-
mon borosilicate glass. p-terphenyl can be used for pulse
shape discrimination between heavy ions, neutrons, and
beta particles [Yanagida et al. 2015]. The response of
p-terphenyl to neutrons and gamma rays is shown in
Fig. 13.40. A study with p-terphenyl in a composite
scintillator in which the organic crystal was mixed into a Figure 13.39. Emission spectrum from crystalline p-
polymer matrix, outperformed composite trans-stilbene terphenyl. Data are from Sangster and Irvine [1956].
Sec. 13.3. Organic Scintillators 537

(a) (b)

Figure 13.40. (a) Scintillation decay response in p-terphenyl from gamma rays and neutrons. (b) Histogram of
gamma ray and neutron events versus the fast/slow integrated signal ratio for Δtf = 20 to 30 ns and Δts = 30 to
150 ns. Data are from Yanagida et al. [2015].

mixtures for neutron/gamma-ray PSD [Iwanowska et al. 2011]. Further, p-terphenyl can be used as the solute
in a liquid scintillation cocktail [Brooks 1956]. The absorption and emission spectrum of such a cocktail is
shown in Fig. 13.41.

13.3.3 Liquid Scintillators


For many radiations the energies of the particles are too small to be measured by conventional means
discussed up until this point. For instance, β-particle emissions from tritium (3 H) have a maximum energy
of 18.59 keV, and the maximum energy of β-particles from 14 C is 156.47 keV. The energies emitted from
these β-particle emitting sources are generally insufficient to penetrate the enclosure of most radiation
detectors, including gas-filled detectors with thin BoPET windows. Sample preparation can also inhibit
detection from energy self-absorption of the radiation particles within the sample. Although some of these
radiations can be detected in a 2π or 4π gas-filled pro-
portional counter, the detection method of choice is
presently a technique referred to as liquid scintillation
counting (LSC), can be used to measure α- and β-
particle emissions, positrons, Auger electrons, internal
conversion electrons, and Compton electrons.
The measurement method involves mixing a radioac-
tive (typically aqueous) sample with the organic scin-
tillation solution. The organic scintillation solution is
commonly referred to as a “cocktail”, and is composed
of a solvent, a surfactant emulsifier and one or more
fluors. The primary fluor is added to convert absorbed
energy into fluorescent light. At times it is beneficial
to mix a wavelength shifting scintillator, or secondary
scintillator, into the solution to improve the scintillation
response. Common fluors and solvents are listed in Ta- Figure 13.41. Absorption and emission spectra from p-
terphenyl dissolved in cyclohexane and fluoresced with 303
bles 13.5 and 13.6, respectively. nm light. Data are from Berlman [1971].
538

Table 13.5. Chemical Formulas and Structures of a Few Organic Liquid Scintillation Fluors (solutes).

Fluor Type Formula Structure

p-Terphenyl primary C18 H14

N
PPO primary C15 H11 NO
O
N N
POPOP wavelength shifter C24 H16 N2 O2
O O

H3C CH 3
N N
M2 -POPOP wavelength shifter C26 H20 N2 O2
O O
N N
PBD primary C20 H14 N2 O
O
CH 3 N N
tert-Butly-PBD primary C24 H22 N2 O H3C C
O
CH 3

H3C

CH 3
bis-MSB wavelength shifter (CH3 C6 H4 CH=CH)2 C6 H4
Scintillation Detectors and Materials
Chap. 13
Sec. 13.3. Organic Scintillators 539

Table 13.6. Chemical formulas and structures of a few liquid organic scintillator solvents when mixed with 3 g/liter PPO.

Solvent Chemical Chemical Relative


Formula Structure Light Yield*

p-Xylene C8 H10 H3C CH 3 1.12

CH 3
Pseudocumene C6 H3 (CH3 )3 1.12
H3C CH 3
CH 3

m-Xylene C8 H10 1.09


CH 3
CH3
o-Xylene C8 H10 0.98
CH3

Xylene (mixed) C8 H10 1.07

Phenylcyclohexane C12 H16 1.02

Toluene C7 H 8 CH 3 1.00

CH3
Ethylbenzene C8 H10 0.96

H3C CH3

Triethylbenzene C6 H3 (C2 H5 )3 0.96

H3C

CH3
n-Butylbenzene C10 H14 0.88

Benzene C6 H 6 0.85

Anisole C7 H 8 O OCH3 0.83

CH 3

Mesitylene C6 H3 (CH3 )3 0.82


H3C CH 3
CH 3

Cumene C6 H5 CH(CH3 )2 CH 3 0.80

CH 3

CH 3
p-Cymene CH3 C6 H4 CH(CH3 )2 0.80
H3C

*As compared to toluene.


540 Scintillation Detectors and Materials Chap. 13

Liquid Scintillation Counting


The solvent serves as a suspension for the primary scintillator fluor; hence, the fluor must be soluble in
the chosen solvent. The excitation energy of the solvent should be relatively low, thereby allowing efficient
transfer of energy to the solvent from the radiation particles. Further, there must be efficient energy transfer
from the solvent to the fluor in order to maintain efficient light output. Historically there are several solvents,
termed “classical” solvents that have been used to great success and consist mostly of the aromatic organic
benzene derivatives (see the list in Table 13.6). Aromatic organic molecules, such as toluene, p-xylene and
m-xylene, have high densities of electrons, thereby producing efficient interaction between β-particles and
molecular electrons so as to generate a relatively large light yield when mixed with a scintillation fluor.
However, these same aromatic hydrocarbons have multiple health risks. Typically they are flammable with
a low flash point (<50◦ C), pose an inhalation problem and can cause skin irritation with direct contact.
Further, there is evidence that benzene and some associated aromatic hydrocarbons cause bone marrow
failure and can lead to forms of cancer involving blood cells (such as leukemia), consequences which have led
to stricter regulations regarding their use.
Until only a few decades ago, scintillation cocktails were usually mixed by the radiation practitioner.
However, in modern times, premixed proprietary cocktail solutions are commercially available from ven-
dors such as Beckman Coulter, Perkin-Elmer, Fisher Scientific, MP Biomedicals, National Diagnostics, and
Research Products International. In recent times, most of these aromatic hydrocarbons, except, perhaps,
pseudocumene (1,2,4-trimethylbenzene), have been replaced with safer solvents. However, pseudocumene
continues to be used in a variety of commercially available “classical” cocktails. An alternative branch of
solvents, named “safer” solvents, are in common use for LSC, considered safer because the safety aspects
to these alternative solvents are safer than traditional classical aromatic hydrocarbons. For instance, a few
alternative safer chemical solvents for LSC are benzyltoluene (BT), 1,2-diphenylethane (bibenzyl or DPE),
2,6-diisopropylnaphthalene (2,6-DIPN or DIN), phenyl xylylethane (PXE), and dodecylbenzene, a linear
alkylbenzene (LAB) [Nemchenok et al., 2011], all of which have low vapor pressures with flash points above
140◦ C and are classified as safe for transport and storage.
There are many benefits to adding a wavelength shifting fluor to the cocktail [Schram 1963]. First, the
emission wavelengths of many primary fluors have sufficient energy to be significantly reabsorbed in the
cocktail solution. The wavelength shifter converts light to lower energies, thereby reducing the probability
of reabsorption. Second, a wavelength shifter can be selected that emits photons that match well to the
light collection device such as a PMT. For instance, a solution with p-terphenyl as the primary scintillator
with λmax near 340 nm may have a wavelength shifter added, such as POPOP with λmax near 410 nm and
this improves transparency with a better match to a common bi-alkali PMT. Third, the longer wavelength
photons are less likely to be absorbed by the container structure, such as the vial walls that contain the
cocktail. Fourth, the longer wavelength photons (λ > 400 nm) are more effectively reflected by TiO2 , a
Lambertian reflector often used in scintillation counting. Typically, wavelength shifting fluors have lower
solubility in the solvent than the primary fluor, hence the reason for their exclusion as a primary fluor.
However, the energy transfer process between fluors requires only a small fraction of wavelength shifter, on
the order of 1% concentration of the primary fluor. Energy lost during the energy transfer process between
primary and wavelength shifting fluors is more than made up for by the improved luminescent transparency
in the cocktail and efficient light coupling to the PMT (or other light sensitive device).
Details on liquid scintillation solutions and measurement methods can be found in several excellent books
on the topic such as those by Ross, Noakes, and Spaulding [1991] and L’Annunziata [2012]. Here, only a
brief overview of the art is presented.

Scintillator Vials LSC systems have conveyer systems that may consist of a belt with vial slots or racks
capable of holding approximately 10 vials. Systems are designed for several vial sizes ranging from 4 ml to
Sec. 13.3. Organic Scintillators 541

25 ml capacity, although the most popular size seems to be 20 ml vials. The 20 ml size became the standard
size limit mainly because of conventional photomultiplier tube diameters. A study conducted with 7 ml and
20 ml indicates that there is little difference in performance using either size of vial [Moore et al. 1977],
although efficiency was better for low energy beta particles (3 H) for the 20 ml vials. It was determined that
use of either should be filled more than halfway to reduce problems with quenching. Overall, the lower cost
of operating with 7 ml vials seemed to be the main consideration. These vials have caps that include either
a white Lambertian or a specular internal reflector.
These LSC vials are available fabricated from several different materials, including quartz, soda lime glass,
borosilicate glass, polyethylene, polypropylene, nylon, and Teflon [Peng 1977]. Quartz has low background
concentrations and is optically clear for UV light emissions, making it a preferred choice for vials. However,
quartz vials are also relatively expensive, and are seldom used for routine samples. Borosilicate glass has a
lower background, mainly from 40 K, than soda-lime glass and is optically clear, thereby making it a good
choice. Further, glass is chemically inert to the organic compounds usually used in LSC. However, glass
does adsorb a variety of other chemicals, including lipids, cations, anions, amino acids, polyethylene glycol,
and many other compounds with hetero-atoms [Peng 1977]. Various additives and surface treatments can
be used to reduce chemical adsorption in glass vials. Polyethylene vials do not appear to suffer from these
adsorption effects. Glass can break, which has the risk of contaminating the workspace and counting system.
Further, it is possible for radioactive particles to fluoresce the glass, which ultimately adds to the background
light output. Finally, glass vials can be costly; therefore, many labs choose to clean used vials rather than
dispose of them.
Polyethylene vials are more economical, but some of the solvents used in LSC can cause plastic vials
to swell (mainly toluene and xylene) which can cause vials to become lodged in a system. Further, the
continuous change in the cocktail solution because of diffusion of the solution through the vials causes a drift
in the measured light output over time. To reduce risk of solvent loss and vial swelling, cocktails with volatile
solvents contained in plastic vials are best measured within a day of preparation. Swelling is less of a problem
with high density polyethylene (HDPE). Polypropylene vials suffer similar problems as polyethylene vials.
Also, there are polypropylene vials available with internal anti-diffusion coatings that effectively reduce this
problem. Polyethylene vials can have higher light transmission efficiency than glass for wavelengths between
360 and 400 nm, and they do not have the risk of breaking. Antistatic plastic vials are available if static
electricity is a concern.
Nylon vials can soften with water-based or alcohol solutions, but are relatively resistant to toluene. Teflon
vials are also inert to chemicals used for LSC, but are more expensive than nylon or polyethylene. Teflon
vials also have a lower radiation background than glass, quartz, and polyethylene vials.

Radiation Measurement Laboratory LSC systems are configured in coincidence mode, such that a cock-
tail sample is inserted between two photomultiplier tubes (PMTs) gated to allow a ‘count’ only when
both PMTs produce a signal above a discriminator setting within a defined time window Δt. The in-
tensity of light, or electrical signal, is a relative measure of the energy deposited within the scintil-
lator. Operating in coincidence mode reduces sporadic background counts from cosmic rays or other
background radiations that may interact directly with either of the PMTs. To further reduce back-
ground, laboratory LSC systems have an abundance of lead shielding28 surrounding the PMTs and
internal source (if there is one). Laboratory units are designed to handle numerous samples in se-
quence. An operator can load hundreds of vials into racks or a conveyor, and each sample is systemat-
ically inserted between the PMTs, and the system automatically records data from each of the samples.

28 One of the authors nearly crushed a perfectly good hand-cranked lift by raising a small Beckman laboratory LSC from the
bottom floor of his lab to a second floor loft area.
542 Scintillation Detectors and Materials Chap. 13

The pulse height spectrum energy from a LSC is usu- 32


P
ally projected onto a logarithmic scale along the abscissa 14
C
(channel number). This arrangement becomes necessary
when comparing low and higher energy beta particle
emissions that are significantly different such as those 3

Counts
H
from 3 H and 14 C. In Fig. 13.42, pulse height spectra
from three common beta particles sources are shown
(3 H, 14 C, 32 P) with maximum energies of 18.3 keV, 156
keV, and 1.71 MeV, respectively. Each spectrum ranges
from zero up to the end point energy, a consequence of
the beta particle always sharing energy with an anti-
Channel Number or Pulse height
neutrino decay product. Because the anti-neutrino does (log[energy])
not produce scintillation light, only the energies from
Figure 13.42. Depiction of output spectra from three
beta particles are recoded in the spectrum. beta particle sources. After [Beckman 1985].

Quench Correction Foreign matter and diluting fluids can cause light loss in a scintillation cocktail. If the
amount of light produced in the scintillator falls below the discriminator setting, then the event is not recorded
by the system. This light attenuation effect is usually categorized as “color” or “chemical” quenching. Color
quenching is a result of chemicals in the solution that change its color and absorb scintillation light. For
instance, yellow coloration produces strong color quenching, whereas blue coloration usually quenches very
little. Chemical quenching occurs when chemicals added to the cocktail interfere with the energy transfer
process and causes inefficient energy transfer to the scintillation phosphor. In either case, the result is a
loss of light, which consequently changes the pulse height spectrum. For example, counts falling within
ch2 in Fig. 13.43 may have 75% efficiency for a low quenched sample, but only 5% efficiency for a highly
quenched sample of the same activity. All LSC samples are quenched and require some amount of quench
correction to determine the actual sample activity. There are many quench correction techniques developed
by LSC manufacturers, and are generally categorized as internal or external standard methods. Some of
these methods are briefly described here.
Internal Standard Quench Correction The internal standard method typically requires that a known
amount of radioactive sample be added to a scintillation cocktail. The sample is initially measured in the
LSC system and afterwards a known amount of radionuclide, generally with high specific activity, is added
to the cocktail followed by another measurement. The efficiency of the standard is determined by,

Cps(s + x) − Cps(x)
s = , (13.42)
Dps(s)

where Cps(s + x) refers to the count rate from the mixed calibrated standard and sample, Cps(x) refers to
the count rate from the sample, and Dps(s) refers to the known activity of the calibrated standard. The
activity of the sample can then be found from,

Cps(x)
Dps(x) = . (13.43)
s
The internal standard method is best used for manual scintillation systems, such as field units, rather
than automated systems. Although the internal standard method is considered accurate, it is time consuming
and impractical for large numbers of samples. Note the method presumes that adding the known standard
to the vial does not affect the overall quench. However, the addition of the standard to the vial changes
Sec. 13.3. Organic Scintillators 543

the total liquid volume and can change the sample quenching, and, consequently, reduce the accuracy of the
measurement. A disadvantage of the method is that the sample cannot be recounted, mainly because the
activity is altered by the addition of the internal standard. Further, opening the vial, especially in a cool
environment, my cause water condensation in the vial, and water is a strong quencher. Also, contamina-
tion from the transfer method (pipette, for instance) can add unintended quench matter into the cocktail.
Addition of these quenches into the sample cocktail lead to exaggerated corrections to the calculated activity.
Internal standards for 3 H and 14 C are commercially available. Typically it is advised to use cocktail
solutions for the radioassay with the composition as the quenched standards. Unquenched standards are
best acquired from commercial vendors, mainly because they are usually flushed with argon to remove
dissolved oxygen. Removal of the dissolved oxygen works to increase the scintillation efficiency. A variation
of the internal standard method includes a unique cap on the vial that systematically pumps a known amount
of calibrated quench fluid into the vial.

Channels Ratio Method LSC is most often used for beta emitting radionuclides; hence the pulse height
spectrum extends from zero up to the maximum energy of the beta particles and the spectrum is very similar
to the beta-particle energy distribution. If the pulse height spectrum is divided into two channels, then the
ratio of counts in the channels can be used to determine the amount of quenching. An advantage of the
method is that no additional standard need be added to the samples, and these samples can be recounted
many times.
The LSC system usually has two independent chan- no
nels, as shown in Fig. 13.43. Many ratio variations can low quench
be used, and do yield different results [Horrocks 1974]. quench
For instance, the numerator may be ch 1, while the de- high
quench 75%
nominator is ch 2, or the numerator may be ch 2 while
the denominator is the sum of ch1 and ch 2, and so on.
Counts

The ratio choice should be selected so that the experi- 5%


mentally determined ratio does not produce a value close
to zero.
The channels ratio quench correction method is per-
formed by initially measuring a set of quench correc-
tion standards. These standards have a specific ra-
dionuclide of interest in the cocktails, 3 H or 14 C for in- ch1 ch2
Discriminator Level
stance, and each standard has a different level of quench
agent added. At least one of the standards remains un- Figure 13.43. Depiction of output spectra from un-
quenched. With the unquenched standard, a measure- quenched and quenched standards used for the channels ra-
tio calibration. The number of counts in channel 1 increase
ment is conducted and the channels set at specific lo- with quenching, while the number of counts in channel 2
cations to split the spectrum into two portions. These decrease with quenching.
channels remain unchanged for both the calibration and
sample measurements. The remaining standards are measured, and the number of counts registered in both
channels are recorded for each measurement.
The known activity of the unquenched standard is compared to the total counts summed from channels
1 and 2. This same exercise is repeated for all standards in the set. The channels ratio (for example,
ch 1 divided by ch 2) is plotted against the counting efficiency for each measurement, thereby providing
a characterization curve for the radionuclide samples. For each unknown sample, the ratio of ch1/ch2 is
determined and compared to the calibration graph, which yields the efficiency. The corrected activity is
then determined with Eq. (13.43).
544 Scintillation Detectors and Materials Chap. 13

ch1 ch2 ch1 ch2

unquenched highly
quenched unquenched
Counts

Counts
quenched (a) (b)

Discriminator Level Discriminator Level

ch2/(ch1+ch2) ch2/(ch1+ch2)
Efficiency (%)

Efficiency (%)
ch2/ch1
ch2/ch1
ch1/ch2

ch1/ch2

CR CR

Figure 13.44. Counting efficiency as a function of the channels ratio for two different
discriminator settings. In example (a) both channels are set relatively high, while a
greater separation is between channel settings in example (b).

Proper selection of the channels is critical to this quench correction method. Consider the two examples
shown in Fig. 13.44. The channel selection of Fig. 13.44(a) causes the counts in channel 2 to approach zero
at relatively low quench. In other words, selection of the channel ratio method causes the ratio to either
approach zero or infinity at a low amount of quench. Although it provides detail in the quench curve for
low quenched samples, it has no information for highly quenched samples. For the channel selections of
Fig. 13.44(b), the spectrum is more evenly distributed, thereby allowing the calibration of quench curves
over a broader range of quenched solutions.
External Standard Method The basic external standard has a gamma-ray source of known activity, usually
a 137 Cs source, as a component in the LSC system. This gamma-ray source (sometimes called a “pea”) is
withdrawn into a shielded region inside the LSC system to prevent unwanted background in a scintillation
cocktail sample. With a sample in the system, the gamma-ray source is withdrawn from the shield and
produces a Compton scattering continuum of energetic electrons in the scintillation cocktail, which adequately
mimics the fluorescent yield of beta particles. The original method proposed by Higashimura et al. [1962]
used the observed count rates and efficiencies from a set of known beta particle standards. For each quench
standard, the counting efficiency is determined by,
Cps(Si )
i = , (13.44)
Dps(Si )

where Cps(Si ) is the count rate for standard i and Dps(Si ) is the known activity of standard i. Each of these
standards, immediately after (or before) the measurement, is exposed to the external standard gamma-ray
source and the new count rate is recorded. This gamma ray source is placed in the same location with
respect to the vial for each measurement. An efficiency calibration curve is developed using the net count
Sec. 13.3. Organic Scintillators 545

rate response from the gamma-ray source,

NCps(i ) = NCps(γ) = Cps(Si + γ) − Cps(Si ), (13.45)

where Cps(Si + γ) is the observed count rate with both the gamma-ray source and the activity of the
LSC standard. The LSC standard efficiency i is plotted versus NCps(γ). For an unknown beta particle
sample, the LSC sample efficiency is found by comparing the measured NCps(γ) against the calibration
curve. Afterwards, Eq. (13.43) is used to determine the sample activity. Note that it is important that all
measurements are conducted for the same amount of time, and that the lower level discriminator is also kept
constant during a set of measurements. Calibration sets can be acquired for different beta particles sources,
the most common being 3 H, 14 C, and 36 Cl to cover low, medium, and high energy beta particles, respectively.
Calibration sets usually have ten quench vials to a set, typically with one “unquenched” standard.

External Standard Channels Ratio Method As the name implies, the external standard channels ratio
(ESCR) method combines an external gamma-ray source measurement with the channels ratio quench cor-
rection method. In a system with ESCR, there are three wide channels. One channel spans the beta particle
spectrum. The other two channels are set higher than the beta particle spectrum, and are used to establish
a quench calibration curve with the external gamma-ray source. Hence, the efficiency of the beta particle
standard is plotted versus the channels ratio of the gamma-ray source. During a measurement of a beta
source of unknown activity, the channels ratio is determined by the gamma-ray source and the beta particle
activity is corrected from the quench calibration curve. As with other techniques, two measurements per
vial must be conducted so as to subtract the beta particle counts from the gamma-ray spectrum.
Although the ESCR method is convenient, making it popular, its accuracy is less than either the channels
ratio or external standard methods [Peng 1977]. Sources of error include dissimilar spectra between the beta
particles and the gamma rays, drift in pulse height (mainly with polyethylene vials), vial thickness differences
between the set of standards and the samples, and solution volume differences.

Pulse Height Spectrum Shift (H-Number) Method A quench method developed by Horrocks [1964] uses
the inflection point of the Compton spectrum for quench identification. Instead of comparing the total counts
in the gamma-ray spectrum from the external source, the endpoint channels of the Compton spectra from
a multichannel analyzer are compared. Consider the Compton spectra of Fig. 13.45. The endpoint energy,
typically designated as the inflection point at the end of the Compton continuum, moves to lower channels in
the pulse height spectrum as the quench increases. The maximum energy transferred from a single Compton
scatter is 477 keV for 137 Cs gamma-rays. Hence, the LSC system is calibrated such that an unquenched
sample exposed to 137 Cs has the inflection point channel aligned with 477 keV. Quenched samples cause the
inflection point to appear in a lower channel.
A quench curve is derived in a similar fashion as the external standard method, in which a set of quench
standards is used, except now it is the difference in the inflection point channel that is correlated to the
efficiency instead of the total counts. This difference in inflection point is defined as the “H number” (after
Horrocks who developed it), where

H-number = Ch(unquenched) − Chi (quenched). (13.46)

The efficiency of each vial in the set of standards is determined from Eq. (13.44), and is plotted versus the
corresponding H-number for each calibrated vial in the set. For an unknown beta particle sample, the LSC
sample efficiency is found by comparing the measured H-number against the calibration curve. Afterwards,
Eq. (13.43) is used to determine the sample activity. Note that the H-number method does not require
that the beta spectrum be subtracted from the Compton spectrum because only the end point in Compton
546 Scintillation Detectors and Materials Chap. 13

unquenched

H# = ch2 - ch1
high
quench
Counts

inflection
inflection point
point

ch1 ch2
Channel Number or Pulse height

Figure 13.45. Depiction of different Compton spectra from a LSC system to


determine the H-number.

continuum matters for the measurement.29 Provided that sufficient counts are accumulated in the Compton
continuum to produce meaningful data, the counting time can be varied between samples. The efficiency as
a function of H-number changes tremendously for 3 H (18.3 keV) and 14 C (156 keV) beta particle sources.
However, for high energy beta particles, such as for 32 P (Emax = 1710 keV) shown in Fig. 13.46, are less
affected by quenching.

13.3.4 Plastic Scintillators


Initially introduced in 1950 by Schorr and Torney, plastic scintillators are in many ways similar to organic
liquid scintillators in composition. Plastic scintillators contain both primary and secondary fluors in a
solvent base that is subsequently polymerized to produce a plastic. This solvent may consist of a monomer
that is polymerized by heating or by the addition of a solidifying catalyst. The first such reported plastic
scintillators were produced by either introducing p-terphenyl into a hot solution of polystyrene (C8 H8 )n ,
which was subsequently allowed to cool and solidify or, alternatively, by adding the catalyst 1% benzoil
peroxide into a solution of styrene and fluors [Schorr and Torney 1950]. In like manner, methods of producing
plastic scintillators from polyvinyl toluene [Koski 1951; Swank and Buck 1953; Buck and Swank 1953],
2,4-dimethylstyrene [Sandler et al. 1960]; and from polymethylmethacrylate (PMMA) [Kienzle et al. 1975;
Klawonn et al. 1982; Salimgareeva and Kolesov 2005] were developed. Buck and Swank [1953] show that
purity of starting materials has a profound effect upon luminosity, with clean and fresh chemicals producing
higher light yields.
Contamination from air and the use of some catalysts that assist with polymerization degrade light
yield. Removal of contaminants is performed by vacuum distillation of the starting materials. Fischer [1955]
describes a method of passing nitrogen through the monomer solution before polymerization. If the plastic
scintillator is not properly processed such that the monomer is completely polymerized, Pichat et al. [1953]
showed that aged specimens have long-term oxidation that led to light self-absorption and reduced luminosity.
It has also been reported that the process temperature to form plastic scintillators can significantly affect

29 This convenience requires that the maximum beta particle energy is well below 477 keV. Otherwise, the beta particle counts
still must be subtracted to ensure that the inflection point is properly identified.
Sec. 13.3. Organic Scintillators 547

Figure 13.46. Calibration efficiency curves from a commercial LSC as a


function of H-number for 3 H, 14 C, and 32 P beta particles. Data are from
[Beckman 1985].

light yield [Basile 1957; Funt and Hetherington 1959]. Further, there is indication that light yield decreases
for polymer molecular weights below about 100,000, becoming strongly dependent on molecular weight below
50,000 [Funt and Hetherington 1959].
Modern commercial plastic scintillators are based on similar chemistry, but the actual types and con-
centrations of primary and secondary fluors are kept proprietary. A casual glance at the varied types and
specifications of plastic scintillators listed in Table 13.3 illustrates the variations in performance that can be
achieved. Many of the legacy plastic scintillators originally developed by Pilot Chemical Co. and Nuclear En-
terprises, Inc., are still being produced by contemporary vendors. Polyethylene naphthalate (poly(ethylene
2,6-naphthalate) or PEN) is a recently reported polymer capable of emitting scintillation photons without
the assistance of fluor additives [Nakamura et al. 2011]. It has a light yield of about 10,500 photons/MeV
with a λmax of 425 nm. The density of PEN is 1.33 g cm−3 and has a refractive index of 1.65 that yields a
critical angle of 65.4◦ at a glass interface. The simplicity of PEN can potentially offer a low cost alternative
to traditional plastic scintillators.
Plastic scintillators have multiple advantages, namely they can be fabricated or machined into a variety
of different shapes, they are relatively inexpensive, they are chemically stable and nonhygroscopic, and they
are relatively fast (τf of about a few nanoseconds). The emission wavelengths are designed to couple well
to conventional PMTs (λmax near 425 nm). The refractive index for most commercial plastic scintillators
is around 1.58, which yields a critical angle of 71.7◦ at a glass interface. Commercial plastic scintillators
have a mass density of 1.038 g cm−3 . Many plastic scintillators also have a long decay component, similar
to organic crystals, and can be used for PSD between neutron and gamma-ray events. The interaction
efficiency of radiation particles can be increased by loading plastic scintillators with additional absorbers.
For instance, neutron interaction rates can be increased by loading the monomer solution with 10 B, 6 LiF, or
Gd. Gamma-ray interactions can be increased by loading the monomer solution with Pb or Sn. There is, of
course, a limit to the amount of additional material that can be added, or otherwise the added material can
548 Scintillation Detectors and Materials Chap. 13

decrease the luminosity of the plastic. Another notable use for plastic scintillators is that it can be used as
a fast neutron detector with special plastics designed for PSD. Because they are composed of hydrogenous
material, they can perform as fast neutron detectors through (n, p) reactions.
The multiple shapes and sizes of plastics include fibers and thin sheets. Scintillating optical fibers can
be used to detect radiation and subsequently transport the luminescent signals relatively long distances to
a light detector. The plastic fibers are typically composed of polystyrene with a refractive index of 1.58.
In order to facilitate light propagation over long distances, a cladding material with lower refractive index
must be applied to produce internal reflection. For instance, PMMA (n = 1.49) or fluorinated PMMA (n =
1.42) are often used as cladding materials. Plastics can also be manufactured as ultra-thin slices. These
thin detectors are thin enough to allow the passage of relatively heavy charged particles, attenuating only a
small portion of energy; hence can be operated as ΔE detectors for heavy ions such as protons and alpha
particles. Thin film organics scintillators are available commercially, some with a thickness as low as 0.25
microns (see Table 13.3).
Recall that Birks’ hypothesized non-linearity in light yield was due to damage by heavy ions, and indeed
radiation damage can be of concern for plastics used over extended periods of time or in high dose environ-
ments. Over time, radiation damage, manifested as broken molecular bonds, cause a decrease in light yield.
The effect may be directly due to damage of the base material, the primary fluor, or secondary fluors, and
either the light emission is decreased or the transparency is decreased from internal absorption. Bross and
Pla-Dalmau [1992] report that plastics operated in air (oxygen) are more affected by radiation damage than
those operated in an inert atmosphere, and they hypothesize that oxygen reacts with radical species formed
under irradiation as it diffuses into the plastic, and that these oxidation products contain carbonyl and hy-
droxyl groups which absorb at longer wavelengths and decrease transparency. Bross and Pla-Dalmau [1993]
also report on radiation hard 3-hydroxyflavone (3HF) polystyrene plastic scintillators that had about 10%
light loss after 10 Mrad of radiation exposure with 137 Cs. Studies performed by Vasil’chenko et al. [1996] on
numerous (about 70) different polystyrene plastic scintillator formulations indicate that radiation hardness
can depend upon the fluor type. Plastics that also contained plasticizers seemed to have higher radiation
resistance, some withstanding little change after an exposure of 7 to 9 Mrad of gamma radiation from 137 Cs.
Alternative polystyrene plastics were studied by Senchishin et al. [1995], who found that radiation hardness
can be improved by the addition of diffusion enhancers (such as diphenyloxide). They also conclude that
plastics prepared with polystyrene pellets rather than a monomer have superior radiation hardness.

13.4 Gaseous Scintillators


Fluorescence in air has been observed by humans living in northern and southern latitudes for millenia.
However, the origin of the northern lights or aurora borealis or of the southern lights or aurora australis
was unknown until the twentieth century. Protons and electrons emitted by the sun are usually deflected by
earth’s magnetic field. But at both poles the magnetic field is weaker and these charged particles can reach
earth’s atmosphere where they excite oxygen and nitrogen atoms and molecules. At high altitudes up to 200
miles the solar wind interacts with atomic oxygen producing 630.0 nm (red) light, but at lower altitudes the
630 nm emissions are suppressed and 557.7 nm (green) emissions dominate. Both the 557.7 and 630.0 nm
emissions correspond to forbidden transitions of atomic oxygen and have decay constants of 0.7 s and 107 s,
respectively. Thus, the red and green emissions are really phosphoresence. At even lower altitudes atomic
oxygen is uncommon and the solar wind interacts with molecular nitrogen and excited molecular nitrogen to
produce light in both the red and blue parts of the spectrum with 428 nm (blue) dominating. That air can
be made to fluoresce by radiation particles is shown dramatically in Fig. 13.47. Monoenergetic deuterons
emerging from the cyclotron travel in almost straight lines and have a well-defined range as can be seen from
the abrupt ending of the fluorescent plume.
Sec. 13.4. Gaseous Scintillators 549

Figure 13.47. The white horizontal misty line is a beam of deuterons emerg-
ing from the 60-inch cyclotron at Argonne National Laboratory. The beam is
visible because of excitation of air molecules by the energetic deuterons. From
Kernan [1969].

13.4.1 Development of Gas Scintillator Counters


Discussed in Chapters 9 through 11 are three basic types of gas-filled detectors that operate on the concept
of induced current from charge collection. Note that gas-filled detectors also release photons through deex-
citation. Ordinarily these photons are purposely quenched to suppress the formation of additional electronic
pulses. However, when the gas is used as a scintillator, this light quenching is undesirable.
The development of the first gas scintillation counter is generally credited to Grün and Schopper [1951];
however, the initial discovery of gas scintillation is not so well defined. It appears that the earliest mention of
radiation induced luminosity from gas was reported by Huggins and Huggins [1903a; 1903b; 1905; 1906] who
studied alpha particle induced (from radium bromide) luminosity from nitrogen, hydrogen, and air. They
deduced that the familiar glow from the radium salt is actually caused by the fluorescing of the surrounding
gas. Numerous studies were conducted on the emission spectra from various gases in the intervening years
between the work of Huggins and Huggins and that of Grün and Schopper. These investigations are briefly
described by Birks [1964]. Grün and Schopper [1951] used purified gases, H2 , Ar, N2 , O2 , and CO2 , which
were irradiated with alpha particles, and the light emissions were monitored with a commercial PMT. They
noted that impurities, including organic gases, caused a decrease in luminosity.
Gas scintillation detectors have some advantages over other types of detectors, especially when used to
detect heavy ions. Gas scintillation detectors are relatively fast, usually having decay times on the order of
a few nanoseconds. They also have a proportional response to energy deposition by heavy ions, an attribute
generally not shared by other types of scintillators (organic and most inorganics). Multiple authors, outlined
by Birks [1964], report a proportional response to charged particles over a wide range of stopping powers
−dE/dx regardless of the radiation type, and that the proportionality is superior to other scintillators (solid
or liquid). Another important attribute is that gas scintillation detectors can be constructed in large sizes,
which can be challenging to produce with solid-state scintillation and semiconductor detectors. Hence, for
550 Scintillation Detectors and Materials Chap. 13

large, fast, and proportional detectors needed for the detection and energy spectroscopy of heavy ions, gas
scintillation detectors may be a good choice.

13.4.2 Theory of Gas Scintillation Counters


The luminescent quantum efficiency, described by Stern and Volmer [1919], and modified by Birks [1964],
can be expressed as follows. From the ideal gas law,
pa V na RT
= , (13.47)
pV nRT
where T is the absolute temperature, R is the gas proportionality constant, V is the volume, and pa and
na are the pressure and molar concentration, respectively, at STP. Rearrangement of terms, the molar
concentration n of gas molecules for a closed container (V = constant) at constant temperature is
na p
n= . (13.48)
pa

Stern and Volmer [1919] express the luminescent efficiency, without collisional quenching, as

kf
1 = , (13.49)
kf + ki
where kf is the rate constant for luminescent emissions and ki is the internal quenching rate constant both
with units of s−1 . The mean decay time is then
1
τ1 = . (13.50)
kf + ki
Birks [1964] adds the product nkc to describe the quenching loss rate caused by collisions.30 With
collisional quenching, Eq. (13.49) is modified as

kf 1
 = = . (13.51)
kf + ki + nkc 1 + p/p
where p is defined as
pa (kf + ki )
p = . (13.52)
na kc
Eq. (13.51) indicates that at low pressures, the intrinsic properties of fluorescence and quenching dominate
the luminous efficiency, while at high pressures the collisional quenching becomes important and possibly
dominant. A similar effect can be observed with the luminescent mean decay time
1 τ1
τ = = . (13.53)
kf + ki + nkc 1 + p/p

With the above formulation for luminescence efficiency, the light yield for a gas can be computed as
follows. Given a specific volume, the total number of ion pairs produced by a charged particle with energy
E is
E
Nion = , (13.54)
w
30 The unit dimensions of kc are not those of ki and kf , but must also include a factor to account for the gas density or pressure.
Sec. 13.4. Gaseous Scintillators 551

where w is the average energy required to produce an ion pair. The value of w is intrinsic to the gas atom
(or molecule), and is not a function of the gas density. The number of ions produced for a partial energy
loss ΔE is
 ΔE
Nion = . (13.55)
w
Hence, the scintillation yield per partial energy ΔEi deposited is the product of the luminescent efficiency
and the number of ion pairs produced, i.e.,
ΔL  ΔEi
 Ai = , (13.56)
ΔE w
and the average light yield per unit energy is,
1  1 Nion
A= 
Ai = . (13.57)
1 + p/p i 1 + p/p

The light yield from a gas is linear with energy deposition as can be seen from Eq. (13.37). Because ΔE
is proportional to p, the light yield for an energy deposition of ΔE is [Grün and Schopper 1954]
p
ΔL = AΔE ∝ . (13.58)
1 + p/p

This result indicates that at low p the light yield decreases to small values (an intuitive result) and at high
p p the light yield levels off to a nearly constant value. This type of dependence was demonstrated by
Grün and Schopper [1954] for a pure N2 backfilled detector and an Ar + 8% N2 backfilled detector.

13.4.3 Factors Affecting Performance


Grün and Schopper [1954] showed that the spectral response Table 13.7. Properties of some gas scintillators at
can be improved by the addition of a small amount of N2 0.974 atm irradiated with 4.7-MeV α particles.
to an Ar backfilled detector, although they did not observe w λm Decay Light Yield
such a benefit when N2 was added to a Xe backfilled detector. Gas (eV/ion pair) (nm) Time (photons Reference
The reason for the improvement is a shift in wavelength from (ns) per MeV)

the short wavelength UV emission, characteristic of Ar (see He 42.3 390 ≤20 234 K1,B
Table 13.7), to the longer wavelength emission of N2 , thereby Ar 26.4 250 ≤20 234 K1,B

improving spectral matching to a PMT. The wavelength shift Kr 24.1 318 447 K1,B
Xe 21.9 325 787 K1,B
is most probably a consequence of ion collisions transferring N2 35 390 ≤20 170 K1,B
energy from Ar to N2 rather than UV photon absorption and
B: Birks 1964; K1: Koch and Lesueur 1958.
reemission [Birks 1964]. Although there is apparent improve-
ment in response with a slight amount of N2 added to Ar, this result is an artifact of the measurement. In
reality, the total number of photons emitted decreases because N2 acts as a quenching gas; however, the
total number of photons detected by the PMT light sensor used in the study increased. Also shown was that
the presence of O2 in small amounts works to reduce performance of Ar-filled gas scintillators.
Because the wavelengths emitted by almost all noble gases are in the UV range and do not match well
to a PMT response (the exception is He), it is common to employ a wavelength shifter. These λ shifters are
either coated upon the PMT window or upon the chamber walls. Several scintillating wavelength shifters that
have been used including trans-stilbene, diphenylstilbene (DPS), p-terphenyl, p-quaterphenyl, POPOP, and
tetraphenylbutadiene (TPB). Of these, Birks [1964] lists that DPS gives the best results when coupled to Ar,
Kr, or Xe gas scintillators. There are precautions that should be implemented when using organic λ shifters.
In particular, the outgassing of organic vapors contaminates the gas and causes a deleterious quenching
552 Scintillation Detectors and Materials Chap. 13

effect that, consequently, lowers light output. Hence, the λ shifter should have a low vapor pressure to
reduce outgassing, or the system can be cooled to also reduce the rate of outgassing. Alternatively, gas-flow
chamber can be employed in which the scintillation gas is continuously replenished with fresh gas, or instead,
the gas can be filtered and purified in a closed-loop system before re-entering the detector chamber. Finally,
the light sensitivity can be increased by using
PMTs with quartz windows through which the
UV light has better transmittance than that of
common soda-lime or borosilicate glass.
The emission efficiency and decay time are
affected by the gas pressure, as can be seen from
Eq. (13.51) and Eq. (13.53). Further, the purity
of the gas also affects the emission spectrum,
light yield, and decay time. A list of some gas
scintillator values are provided in Table 13.7,
although these values are limited to a specific
case. The complex nature of energy transfer to
luminescent levels in a gas scintillator proves dif-
ficult to model theoretically. However, Koehler
et al. [1974] proposed the use of a summation
of numerous exponential terms to model the
Figure 13.48. Normalized emission intensity for Xe gas as a func- scintillation decay response of Xe and Ar gases.
tion of gas pressure. [Parameters are from Koehler et al. 1974]. They model the emitted light intensity by

I(t) = Ai e−t/τi , (13.59)
i

where Ai and τi are experimentally determined amplitudes and decay constants. The terms Ai and τi are
listed in Koehler et al. 1974 for gas pressures ranging from 0.27 atm to 54.4 atm for Xe and ranging from
6.8 atm to 65 atm for Ar. The time responses for Xe gas at a few selected pressures, based on the work of
Koehler et al. [1974], are plotted in Fig. 13.48.

13.4.4 Mixtures of Noble Gases


Gas mixtures of different noble gases have also been studied [See, for example Northrop and Gursky 1958b;
Thiess and Miley 1974]. In general, the mixing of noble gases causes a decrease in light yield, with a mixture
of He and Xe being the exception. Biondi and Brown [1949], Biondi and Holstein [1951], and Biondi [1952]
propose that the dominating recombination process in a pure noble gas are (1) collisions between atomic ions
and atoms that form stable molecular ions and (2) the subsequent capture of an electron by a molecular ion
produces two atoms in excited states. These excited atoms can release scintillation photons. Apparently, the
electron capture probability of the molecular ion is much greater than that of the atomic ion as suggested
by the observation of significantly greater radiative recombination coefficients for the purified noble gases
[Biondi 1952]. Recall from Chapter 10 (Table 10.6) that the ionization potentials of noble gases decrease with
increasing atomic weight. In a gas mixture, the positive charge is transferred in collisions from the lighter
gas molecule to the heavier molecule because the heavier gas always has the lower ionization potential. With
the addition of small amounts of heavy gas to a lighter gas, the charge is rapidly passed to the heavy gas in a
similar fashion as described for quenching gases in proportional counters. Because the concentration of heavy
gas atoms is lower than in the pure condition, the probability of ion-atom collisions producing molecular
ions is decreased, and consequently, the production of excited atoms is decreased. Consequently, the light
yield typically decreases. The exceptions are a mixture of Xe-He, within a pressure ratio range of about 8%
Sec. 13.4. Gaseous Scintillators 553

to 100% Xe, and a mixture of Xe-Ne, within a pressure range of about 40% to 60% Xe. The optimum light
yield was reported as about 10% Xe in He and yielded over 20% increase in light yield compared to that of
pure Xe [Northrop and Gursky 1958b]. Shown in Fig. 13.49 are light yield curves for different gas mixture
ratios of Xe fluoresced with alpha particles from 234 U. Other gas mixture combinations of He, Ne, Ar, and
Kr produced lower light yield than the Xe mixtures.

13.4.5 Liquid and Solid Noble Elements


The noble elements at high pressures have also
been studied both in the liquid and solid state
phases [see Aprile et al. 2006]. According to
the observations of Simmons and Perkins [1961],
the emission spectrum from liquid He is differ-
ent than that from the gas phase and is in the
far UV region (less than 160 nm) well below
the transmission cutoff of quartz glass (about
180 nm). Similarly, Ar and Xe at high pres-
sures (34 bar) were found to emit light centered
at 126 nm and 169 nm, respectively [Koehler
et al. 1974]. For such high energy UV pho-
tons, caution should be exercised to ensure that
the photons are not reabsorbed in the detect-
ing medium and can pass through the glass en-
closure of the PMT. Consequently, soda-lime,
Figure 13.49. Light yield of noble gas mixtures to that of pure Xe borosilicate and even quartz windows should
gas. Shown are mixtures with the gas pressure fraction of Xe added not be used for the detection of these emissions
to He, Ne, Ar, and Kr. Wavelength shifters were used in the work; because they are effectively absorbed at these
diphenylstilbene for He-Xe, Ne-Xe, Ar-Xe, and p-quaterphenyl for
Kr-Xe. Data are from [Northrop and Gursky 1958b].
short wavelengths. However, the introduction
of a wavelength shifter on the chamber walls
and PMT window can effectively overcome this problem. The results reported by Northrop et al. [1958a]
are listed in Table 13.8 for noble element scintillators when irradiated by alpha particles. Several cases are
shown, including a comparison to NaI:Tl, which lists the use of a UV sensitive PMT (DuMont K1306) and
a common bialkali PMT (DuMont 6292) with and without the assistance of a p-quaterphenyl wavelength
shifter. Light yields from liquid and solid Xe were notably high, with liquid Xe having nearly the same light
response as NaI:Tl and solid Xe having nearly twice the light response as NaI:Tl. Northrop et al. [1958a]
note that the results of Table 13.8 were difficult to reproduce, but do reveal a trend in performance. More
recent results by Doke et al. [1990] confirm Northrop’s earlier work, reporting a light yield of about 4 × 104
photons/MeV for both liquid Ar and Ne. From the work of Kubota et al. [1978] and Hitachi and Takahashi
[1983], fast and slow decay times have been observed for liquid Ar (τf = 6 ns; τs = 1590 ns) and liquid Xe
(τf = 2.2 ns; τs = 27 ns). There is some indication that these decay times change with radiation type, but
the differences reported by Hitachi and Takahashi [1983] were small. However, a relatively large difference
in the light intensity ratio If /Is was reported, with electrons yielding a small ratio (0.05), and increases
for heavy charged particles for which If /Is = 0.45 for alpha particles and If /Is = 1.6 for fission fragments.
Because of the low temperatures required to form liquid and solid noble elements, light coupling can be
challenging. Although PMTs can be used, special models must be used that are capable of operating at
cryogenic temperatures along with possessing enhanced sensitivity at UV wavelengths.
554 Scintillation Detectors and Materials Chap. 13

Table 13.8. Efficiencies of some noble element scintillators irra-


diated with α particles. Properties are normalized as compared
to NaI:Tl without wavelength shifters.
PMT Type DuMont DuMont
→ K 1306 6292

PMT Converter QP None QP None



Reflector Mo Mo Mo Al Mo

Reflector Coat none QP none QP none QP none

Xe
Gas 0.34 0.25 0.74 0.66 0.5 0.55 0.49
Liquid 0.43 0.37 0.92 1.29 0.78 0.52 0.75
Solid 1.00 1.91 0.82 0.85 1.03

Kr
Liquid 0.43 0.43 0.80 1.19 0.86 0.69 0.70
Solid 0.16 <0.04 0.31

Ar
Liquid 0.36 0.37 0.55 0.52 0.46
Solid 0.35 <0.04 0.58

NaI:Tl 0.59 0.97 0.90 0.87 1.00

Reproduced from Northrop et al. 1958 and Birks 1964.


QP ≡ p-quaterphenyl.

13.4.6 Gas Proportional Scintillation Counters


It can be advantageous to apply voltage within the chamber of a gas scintillation detector. With an applied
electric field, the liberated electrons can be drifted through the gas, much like as in an ion chamber. If
the electric field is kept below the critical field required to produce avalanching, then collisions with bound
electrons in the gas can be excited to higher energy levels, but do not produce impact ionization. As these
excited electrons drop through lower states and eventually to the ground state, they lose energy sometimes
by the emission of photons. Hence, this energy transfer produces a type of scintillation light gain. This
operation is the basic principle behind a gas proportional scintillation counter (or gas PS counter) [Policarpo
1977].
An interesting advantage to the gas PS counter is its improved energy resolution over traditional propor-
tional counters. Although the name given to the device is the “gas proportional scintillator counter,” it is
usually not operated in the proportional region of the gas pulse height curve. If operated in the proportional
region, where avalanche multiplication occurs, the statistical fluctuation in electron production increases
above that of the initial density of electron-ion pairs (see Chapter 10). Hence, the fluctuation in light pro-
duction also increases thereby diminishing energy resolution. Policarpo et al. [1972] and Policarpo [1977]
show that the gas PS counter can produce relatively good energy resolution for low-energy photons and for
alpha particles. If a Gaussian model is assumed, the energy resolution of a detector can be approximated by

2 2
FWHM = 2 2 ln(2)E(σeh + σpe + σg2 )1/2 , (13.60)

2 2
where E is the radiation particle energy, σeh is the fractional variance of ionization production, σpe is the
2
fractional variance of photo-electron production, and σg is the fractional variance photomultiplier gain.
Problems 555

Equation (13.60) can be rewritten as,


 √ 2  √  1/2
 F n0 npe 2 σG 2
FWHM = 2 2 ln(2)E + + , (13.61)
n0 npe G

 Fw w σ2
1/2
=2 2 ln(2)E + + G2 ,
E ELc pe G
where the FWHM is in units of energy, F is the Fano factor, and w is the average ionization energy, L is
the light yield at the operating voltage, c is the light collection efficiency, pe is the photoelectron emission
2
efficiency, G is the PMT light collector gain, and σG is the variance in the PMT gain. Typically, the largest
statistical variance in gain is the fluctuation in the initial number of photoelectrons produced, accounted for
in the second term of Eq. (13.62); hence the third term is usually small so that

 F Lc pe + 1
1/2
FWHM  2 2 ln(2)Ew . (13.62)
Lc pe

As previously discussed, noble gas mixtures usually have reduced light yield. However, Alkhazov et al.
[1967] show that optimized mixtures of noble gases can decrease the Fano factor. One can observe from
Eq. (13.62) that a reduction in F improves the energy resolution, while a decrease in L works to degrade
energy resolution; therefore, a proper optimization of the gas mixture should be developed for best results.
There are numerous configurations for the gas proportional scintillation counter [see Aprile et al. 2006
for examples], yet they almost all share a few attributes. The gas chamber has a drift volume designed
with a fairly constant electric field which is adjacent to a high field scintillation region. Interactions in the
constant field drift region produce electron-ion pairs. The electrons are drifted into the high field region
where they gain enough energy to excite more electrons to upper energy levels of the noble gas, but not
enough to produce more ionization (or a Townsend avalanche). The high field region is usually small by
comparison to the drift region, and can be achieved with small diameter anodes in a similar fashion as
in a proportional gas-filled counter. The scintillation light is usually measured with a PMT, although
alternative structures with photodiodes have been explored. Other types of gas proportional counters may
use microstrip or microgap detectors, or even gas electron multipliers (GEMs). In any event, the goal is to
produce scintillations adjacent to a light sensing device with minimal reabsorption loss. As mentioned earlier,
impurities can seriously quench the scintillation process, so gas proportional scintillation counters are usually
operated as gas-flow detectors in which the high-purity gas is constantly replenished. Wavelength shifters
applied to the PMT (or other light collector), and to the chamber walls can help enhance the luminescent
response. Excellent energy resolution has been realized, on the order of 9.7% FWHM for 5.89 keV gamma
rays [Palmer 1975] and 1.6% FWHM for 8.1 MeV alpha particles [Conde and Ferreira 1975].

PROBLEMS
1. Given that Se = Sg and ωe = ωg , derive the result for Eq. (13.9).

2. Determine the light conversion efficiency for NaI:Tl photoelectric absorption 898 keV gamma rays.
Assume the maximum wavelength and light yield from Table 13.1 apply.

3. Prove Eq. (4.58) reduces to Eq. (13.35) for non-relativistic particles (vi  c).
556 Scintillation Detectors and Materials Chap. 13

4. A beam of 1-MeV gamma rays is normally incident on a CsI crystal that is 30 mm thick. What is the
probability that an incident gamma ray has one or more interactions in the crystal?

5. The dead time in a particular scintillator detector is 2 μs and in typical gas-filled detector is 250 μs.
For a particular radionuclide sample, the gross counts obtained with the gas-filled detector suffer a 5%
loss because of dead time. For the same source-detector geometry, what is the loss in the scintillator
detector?

6. Given the task to efficiently detect gamma rays in the 30 to 60 keV range with a size restricted detector
only 2 mm thick, which material would you use given the options of NaI:Tl, GSO, and LSO? Explain
your selection choice.

7. Suppose you have a NaI:Tl detector with 7% FWHM energy resolution when operated with a 1 μs
shaping time at 300K. What is the expected energy resolution if the temperature is increased to 325K?

8. Given a parallel beam of 662 keV gamma rays from a 137 Cs source, compare the efficiency for initial
interactions in 1 cm thick slabs of NaI:Tl, LaBr3 :Ce, and LSO:Ce. What is it for 1.332 MeV gamma
rays for these three scintillators?

9. The best choice of a scintillator material for a detector depends on many factors such as (a) cost,
(b) availability, (c) response speed, (d) response linearity, (e) light output, (f) detector efficiency for
high-energy photons, (g) radiation hardness, and (h) ability to discriminate between different types of
radiation. Evaluate the attractiveness of a typical inorganic scintillator, such as NaI(Tl) and an organic
scintillator, such as a plastic one, with regard to each of above performance factors.

10. Why are organic scintillators preferred for electron and beta-particle detection while inorganic scintil-
lators are preferred for gamma-ray detection?

11. Explain the purpose of adding a trace amount of an activator element to an inorganic scintillator. Why
is an activator not needed in organic scintillators?

12. A set of 10 vial standards, each having an activity of 0.1 μCi 14 C, has the following results for 10 second
measurements in a LSC system:

ch1 ch2
420 26600
1000 23000
1600 20000
2000 17400
3500 13500
4200 11100
5000 8700
5900 6000
6800 3500
7800 1200

You then measure an unknown 14 C sample with 55120 in ch 1 and 106,000 counts in ch 2. What is the
activity and standard error of the unknown sample?
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Chapter 14

Light Collection Devices

We have learnt through experience that when an electrical ray strikes the surface of an atom, an
electron, and in some circumstances a second and even a third electron, can be detached.
Johannes Stark

Scintillators have been used as a method to observe radiation interactions from the time that Röntgen, in
1895, first observed x-ray fluorescence from a plate coated with barium-platinocyanide (BaPt(CN)4 ). Hans
Geiger meticulously counted alpha particle interactions under a microscope, indicated by flashes of light
from a glass slide coated with zinc sulphide (ZnS), a fatiguing technique that inspired Geiger to invent his
famous gas-filled detector alternative [Rutherford and Geiger 1908]. Crooke’s spinthariscope was a more
useful hand-held version of the scintillation/microscope setup used by Geiger. The first hand-held x-ray
imaging fluoroscopes used scintillator screens to view various densities of attenuator for medical purposes.
In fact, for over 50 years since the time Röntgen first discovered x rays, scintillators had been used for some
basic radiation detection purposes. Yet, it was not until the development of a reliable quantitative method
of detecting light emissions, other than the human eye, did scintillators become a standard used in research
and industry for radiation detection and spectroscopy.
A series of discoveries and inventions led to the technologies used today for quantitatively recording
radiation-induced emissions from scintillators. The most popular and widely used of these technologies is
the photomultiplier tube (PMT), which is a vacuum tube that incorporates multiple amplification stages to
produce large signal amplifications through secondary electron emission. Another important technology, also
based on the same idea of the multiplication of secondary electrons, uses microcapillary tubes coated with
electron emissive materials. Finally, a third photosensitive technology is based on excitation of conduction
electrons in a semiconductor solid. An entire book could be written on the design, operation and application
of these technologies to a wide variety of uses; however, that simply is not the goal here. Instead, these basic
technologies, in their various forms, are described in this chapter as they are used in radiation detection and
measurement.

14.1 Photomultiplier Tubes


In 1887, Heinrich Hertz [1887] made the observation that the voltage required to produce an electric arc
between electrodes decreased if assisted by visible light illumination. He also observed that electrical arcing
would also occur only for certain wavelengths of light, regardless of the intensity of light. These observed
effects were later explained by Albert Einstein with what is now known as the photoelectric effect. It was
in 1902 that Austin and Starke [Bruining 1954] published the observation that an electrical current, when
directed onto a metallic surface, could produce a greater number of electrons emitted than those impinging
upon it, a process often referred to as “secondary electron emission.”

565
566 Light Collection Devices Chap. 14

It was J.A. Slepian who first published, as U.S. patents, inventions that used the “Stark effect” to
produce a current amplification device [Slepian 1923]. In the original description, a heated filament provided
a thermionic stream of electrons, guided by magnetic and electric fields into an intermediate anode. Electrons
striking this second electrode would then eject more electrons, thereby causing an increase in current, which
was subsequently collected at another anode. Although the patent drawing is a simple device with only
one electrode producing secondary electrons, Slepian explains that numerous intermediate electrodes can be
inserted to increase the gain further, or in his words, “indefinitely.” The Slepian device is the predecessor of
modern day photomultiplier tubes (PMTs).1
During the 1930s, L.A. Kubetsky also designed several working prototypes of secondary emission ampli-
fiers, all of which were based on Slepian’s original concepts [Kubetsky 1937]. Kubetsky has been credited
with demonstrating the first working electron amplification device, having built the first unit in 1930 [Lub-
sandorzhiev 2006], although these early “Kubetsky tubes” were more closely akin to microchannel plates
than photomultiplier tubes. Various photomultiplier versions were later described by Kubetsky in his 1937
publication as having gains of greater than 103 .
Also, in 1934, Krebs [1934] introduced a type of Geiger-Müller (GM) tube into which a photocathode was
inserted so that the tube could respond to scintillation light. Photons striking the photocathode would eject
electrons, which would subsequently produce a Geiger discharge. By 1941, Krebs had improved the device
somewhat [Krebs 1941; Daggs et al. 1952], although these devices were largely dismissed due to limited
spectral sensitivity. Further, they were mainly based on placing a scintillating ZnS screen near the tube to
produce scintillation light which would then fall on the photocathode. However, such a radiation-to-light
conversion device proved to have limited efficiency for gamma rays, although it worked well for alpha and
beta particles [Daggs et al. 1952].
A chemical process introduced in 1948 by Scherb [1948] extended and improved the spectral response of
the photo-sensitive GM tubes, which seemed to provide a promising method to produce a photo-sensitive
detector for scintillators. Advancements also included the incorporation of scintillation materials as an
integral part of the GM tube [Mandeville and Scherb 1950, Krebs 1955]. Photon-sensitive GM counters were
commercially available during the early 1950s for scintillation counter measurements.2 However, because GM
counters do not preserve energy deposition information, these GM counters could be used only as radiation
counters and could not function as spectrometers.
Meanwhile, work at the Radio Corporation of America (RCA) led to the demonstration of a single
stage electron amplifier based on secondary electron emission that used electric fields to focus and guide
electrons [Iams and Salzberg 1935]. The device had an average gain of approximately 8 and did not receive
much interest. However, continued research on electron amplifiers eventually led to the demonstration of
multistage photomultiplier tubes [Zworykin et al. 1936]. These early PMTs used magnetic and electric fields
to accelerate and direct the electrons, a technique which proved difficult to control.
Some early attempts were made to wed charge amplification with vacuum tube technology [Zworykin and
Rajchman 1939; Rajchman and Snyder 1940], but it was not until 1941 that the RCA Company released
the first commercially successful multistage photomultiplier amplification tube that used secondary electron
emission as the amplification mechanism [Janes and Glover 1941, Glover 1941]. The RCA Type 931, shown in

1 There seems to be some contention regarding the inventor of the PMT, whether it is rightfully Kubetsky [1937] or the RCA
group consisting of Zworykin, Morton, and Malter. Lubsandorzhiev [2006] writes in his short review paper that Zworykin
visited Kubetsky’s laboratory during 1934, implying that Zworykin was inspired by Kubetsky’s work on electron amplifying
tubes, thereby suggesting that Kubetsky is the originator. However, it was Slepian [1923] that suggested the use of multiple
electrodes to increase the gain, as acknowledged by Kubetsky [1937]. Hence, by the authors’ estimation, the fundamental
operation of a PMT was actually first described by Slepian.
2 The Nuclear Research Corp. of Philadelphia, Pennsylvania, for instance, commercialized these photon-sensitive GM tubes.
Sec. 14.1. Photomultiplier Tubes 567

Fig. 14.1, was originally used as a signal amplifier for electronics, in particu-
lar it was used to jam radar during the second world war. Shortly thereafter,
Curran and Baker [1944] reported the use of a PMT placed adjacent to a ZnS
scintillator screen to detect alpha particles. This application is the first reported
use of a PMT for radiation detection. A few years later, Marshall et al. [1947]
demonstrated the use of a PMT wrapped in a fluorescent material to detect x
rays.
Further, Marshall and Coltman [1947] and Coltman and Marshall [1947]
demonstrated the coupling of various different scintillating screens to PMTs to de-
tect alpha particles, beta particles, x rays, gamma rays, and neutrons. That same
year, Broser and Kallman [1947a] also coupled scintillating screens to a PMT to
detect alpha particles, and later that same year reported the use of the organic
scintillator naphthalene with a PMT [Broser and Kallman 1947b]. Throughout
the following few years, numerous groups reported on the advantage of coupling a
light-collection of PMT amplifiers to radiation scintillators. Notably, Hofstadter
[1948] discovered the inorganic scintillator NaI(Tl), which when coupled with a
PMT produced the first practical solid-state gamma-ray spectrometer.
It is the introduction of the PMT that led to the practical realization of
scintillation spectrometer detectors (see articles by Morton [1975a, 1975b]. Even Figure 14.1. The RCA
931A was the first commer-
today a PMT is the most popular light measuring device for most scintillating cially available PMT.
materials, mainly because of their high gain and low dark current.3

14.1.1 Basic Design


The basic design of a photomultiplier includes (1) a transparent envelope, typically constructed of glass, (2) a
photocathode, (3) a series of dynodes, and (4) an anode. Each component, described in the following sections,
plays an important role in the efficiency, timing, and ultimate energy resolution of the spectrometer. The
photomultiplier is a simple device to understand. The basic PMT, depicted in Fig. 14.2, has a photocathode
that is located so as to absorb light emissions from a light source such as a scintillating material. When
photons of light strike the coating on the photocathode, they emit electrons that can diffuse through the
coating to the surface facing the vacuum of the tube. A fraction of these diffusing electrons then escape
the surface and enter the vacuum tube. A voltage applied to the tube guides the liberated electrons to an
adjacent electrode called a dynode. As an electron approaches the dynode, it gains speed and energy from the
electric field formed by the applied voltage. Hence, when it strikes the dynode, it again causes more electrons
to become liberated into the tube. These newly liberated electrons are then guided by the electric field to
the next dynode where more electrons are liberated and so on. As a result, the total number of electrons
released is a function of the number of dynodes in the PMT and the photoefficiency of the photocathode
and the dynodes.
The total charge released in the PMT is
Q = qe N0 GM (14.1)
where qe is the charge of an electron, N0 is the initial number of photo electrons released at the photocathode,
G is the number of electrons released by a dynode per incident electron (the gain), and M is the total number

3 In1941, RCA was the first company to introduce a commercial PMT into the marketplace. The RCA plant, located in
Lancaster PA, was purchased by GE in 1986, whereupon in 1987 the former RCA management team purchased the PMT
facility and technology, forming Burle Industries. Burle was later purchased by Photonis in 2005. Unfortunately, in 2009,
Photonis discontinued the PMT line. ADIT Electron Tubes, a division of Ludlum Measurements Inc., purchased the production
equipment and presently offers PMTs designed primarily for radiation detection.
568 Light Collection Devices Chap. 14

detector window photocathode dynodes


scintillator

anode

g-ray current
output

reflector
scintillation coupling PMT photoelectron vacuum
photons compound window tube

Figure 14.2. The basic mechanism of a photomultiplier tube (PMT). An absorbed γ ray
causes the emission of numerous light photons which can strike the photocathode. A scin-
tillation photon that strikes the photocathode creates a photoelectron. The photoelectron is
accelerated and guided to the first dynode by an electric field, where it strikes the dynode
and ejects more electrons. These electrons are accelerated to the next dynode and excite more
electrons. The process continues through the dynode chain until the cascade of electrons is
collected at the anode whose output current is used to produce a voltage pulse.

of dynodes in the PMT. For instance suppose that a PMT has 10 dynodes each operated with a gain of
4. An event that initially releases 1000 electrons (N0 ) causes over 109 electrons to emerge from the PMT!
Shown in Fig. 14.3 are the components of a NaI(Tl) detector (top) along with a complete detector (bottom).
Also shown in Fig. 14.4 are the internal components of a NaI:Tl scintillation detector.
The photomultiplier tube is an extremely important tool in radiation detection because it is the device
that allowed scintillation materials to become practical detectors. The PMT can take a small amount of
light produced in a scintillator from a single radiation absorption and turn it into a large electrical signal.
It is this electrical signal, typically converted to a voltage pulse, that is measured.
PMTs are stable and electronically quiet (low noise). Modern varieties have exceptional photocathode and
dynode efficiencies, often referred to as the quantum efficiency, with gains that can exceed 30. However, there
is an important design consideration. PMT materials used as photocathodes are generally fabricated from
alkaline metals, which are most sensitive to light with wavelengths in the 350 to 450 nm range. Scintillators
emitting light outside this range can still be used under some circumstances, although their effectiveness can
be severely compromised.

14.1.2 Light Collection and Coupling


So far PMTs are treated simply as light collection devices, with a brief cautionary note about wavelength
matching between the PMT and the scintillation light. In this section, this important aspect in the design
of PMTs is discussed in much greater detail.4

4 Throughout this chapter, “light” is characterized either by its wavelength λ = c/ν or by the energy of its photons E = hν.
To convert between these two characterizations, a useful relation is

λE = hc = 1240 nm eV.
Sec. 14.1. Photomultiplier Tubes 569

Figure 14.3. An encapsulated NaI(Tl) crystal in a reflective canister is shown


in the upper left and a photomultiplier tube is shown in the upper right. The
two components are coupled together to form a scintillation counter such as
the one shown in the lower half. The NaI(Tl) scintillation spectrometer is
composed of a 2×2 inch NaI(Tl) crystal coupled to a PMT, both of which are
sealed in the container together. The combined voltage divider and preamplifier
unit is attached to the back (right side) of the PMT.

Figure 14.4. An x-ray photograph of a 3 in × 3 in NaI:Tl detector coupled


to a linear focus PMT, resistive divider, and preamplifier.

Snell’s Law
The index of refraction is defined as the ratio of light speed in vacuum to that in a particular medium,
c
n= . (14.2)
v
Snell’s Law is a fundamental law describing the reflection and transmission of light at the interface between
two adjacent optical surfaces. This law states, using the notation shown in Fig. 14.5(a),
sin θ1 n2 v1
= = , (14.3)
sin θ2 n1 v2
570 Light Collection Devices Chap. 14

where ni and vi are the index of refraction and the speed of light in medium i, respectively. The index of
refraction for some common window materials is given in Table 14.1.

Table 14.1. Index of refraction (at λ = 410 nm) and cut-off


wavelength below which the transmission is less than 10% of
the maximum.
Window Index of Cut-off
material refraction wavelength (nm)
Soda Lime 1.536 300
Borosilicate 1.530 270
GE 214 (fused silica) 1.459 <160
Suprasil 310 (fused silica) 1.469 <155
Quartz 1.557
Al2 O3 1.785 145
MgF2 1.383 115
LiF 1.398 105

v 1 q1
qc
q q
interface n1 interface n1 interface n1
n2 n2 n2
q2

v2
(a) (b) (c)
Figure 14.5. Snell’s Law showing (a) refraction through two media, (b) total internal
reflection at the critical angle, and (c) total internal reflection beyond the critical angle.
In these figures it is assumed n1 ≥ n2 .

For the case n1 > n2 , θ2 > θ1 as is shown in Fig. 14.5. There is a critical angle in medium 1, for which
θ2 = 90◦ beyond which no light is transmitted into medium 2 and all light is reflected back into medium 1.
This critical angle for medium 1 is
θ1c = sin−1 (n2 /n1 ). (14.4)

However, if n1 < n2 , there is no critical angle for medium 1, i.e., light is transmitted for any incident angle.
Therefore, to reduce light losses from internal reflection at the scintillator/PMT interface, the index of
refraction for the PMT window should closely match the index of refraction of the scintillation material.
Because of a possible index mismatch between many common scintillation materials and PMT windows, a
coupling compound is usually placed between the two materials. Coupling compounds are usually selected
such that ncoupling  nwindow .
Sec. 14.1. Photomultiplier Tubes 571

Example 14.1: Determine the critical angle for light propagating from common glass into air.

Solution:
The index of refraction for air is n2 = 1.0, and glass has an index of refraction approximately equal to
n1 = 1.5. From Eq. (14.4),

θc = sin−1 (n2 /n1 ) = sin−1 (1.0/1.5) = 41.81◦ .

Lambert’s Cosine Law


It is usual for the scintillator to be encapsulated in a
reflecting cannister in which some portion of the can- z
nister has a transparent window for light to exit. For W
best results, the cannister window should have an index
of refraction as close to those of the scintillation mate- n q
rial and the entrance window to the PMT. Further, the
relative amount of light (per unit energy deposited in vacuum
the detector) that enters the PMT from the scintillator dA
material should, ideally, be constant.
Consider a homogeneous half-space (a wall of the
canister, for example) in which there is a constant light y
source emitting isotropically S photons cm−3 s−1 . As y
shown in Fig. 14.6, on the surface (the x-y plane) is a
small area δA whose outward normal is the z-axis. The x
number δN of photons emitted per unit time from a homogeneous
differential volume dV a distance r from δA that pass medium
dW
through δA in a differential solid angle dΩ about Ω is r
 
δA cos θ
δN = S dV exp(−μr). (14.5)
4πr2 dV = dr r 2 dW

Here S dV is the number of photons emitted isotropi-


Figure 14.6. Coordinate system used to describe Lam-
cally from dV per unit time. The term in parentheses bert’s cosine law.
is the probability photons emitted from dV are emitted
towards δA, i.e., the fraction of the total solid angle subtended by δA at dV . The last term is simply the
probability a photon travels to δA without interacting with the medium, which has an interaction coefficient
μ.
The total flow through a unit area on the surface in direction dΩ about Ω from all dV = r2 dΩdr is
 ∞  ∞
S cos θ S cos θ
Jn (Ω)dΩ = (δN/δA)r2 dΩdr = dΩ d−μr dr = dΩ. (14.6)
0 4π 0 4πμ

From this result it is seen that the probability a photon emerges in a unit solid angle about a direction θ is
proportional to cos θ, i.e., the intensity of light emitted from the surface is I(θ) = I(0) cos θ W cm−2 sr−1 .
Any surface emitting light whose intensity is proportional to cos θ is called a Lambertian surface.
572 Light Collection Devices Chap. 14

Lambertian surfaces have an amazing property. As shown in Fig. 14.7, if one views an area A on such a
surface the projected area perpendicular to θ is A/ cos θ cm−2 . The sterance5 or light L observed by the eye
or other light detector is
I(0) cos θ I(0)
L= = . (14.7)
A cos θ A
This means the surface appears equally bright no matter from what angle the surface is viewed. For example,
the surface of the sun is a Lambertian surface, so the sun’s disk appears uniformly bright from the center to
the edge.
The important result of Eq. (14.7) indicates that the sterance
from a Lambertian surface is constant, hence the reflected light from
the cannister walls that reach the transparent interface between the
projected scintillator and the PMT is almost constant regardless of where on
surface area q the surface the reflected photons originated. Such is not true for a
at angle q specular surface, at which the angle of light intersecting the trans-
parent interface is a strong function of the initial location of the
scintillation flash, thereby causing a large variance in the transmit-
surface with area A
ted and internally reflected light. Hence, there is a larger variance in
Figure 14.7. Depiction of projected area light transmitted into the PMT from a specular reflector compared
as a function of angle. to that from a Lambertian reflector.
Because energy resolution depends on the variance of the light entering the PMT, a Lambertian reflector
wrapped around the scintillator produces better energy resolution than does a specular reflector. Common
materials used to produce a near Lambertian surface include Teflon tape, Al2 O3 , TiO2 , and MgO powder.
These materials produce a diffuse light reflection nearly independent of where the initial radiation interac-
tion occurs in the scintillator. The product Spectralon R
, a fluoropolymer, has nearly perfect Lambertian
reflectance for wavelengths between 400 to 1500 nm.
Window Reflection and Transmission
After scintillation light transits the interface between the detector and the PMT, it must still pass through
the transparent PMT window in order to reach the photocathode material. There are a variety of PMT
window materials, each having a short wavelength cutoff beyond which photons with small wavelengths
become strongly absorbed in the window (see Table 14.1). Many scintillators emit wavelengths near 40
nm (400 angstroms), which generally matches well to common glasses, including soda-lime and borosilicate
glasses. However, there are many important scintillators that emit photons with wavelengths in the near
UV region (300-400 nm) and are strongly absorbed by common glasses. The characteristic light response
function of a scintillation detector can be severely compromised at short wavelengths simply by a poor choice
of a PMT window.
Some of the light, with a wavelength λ, that impinges perpendicularly on an interface between two media
undergoes reflection. The fraction of light reflected, or the reflectance, is [Hecht 1987]

[n2 (λ) − n1 (λ)]2


R12 (λ) = . (14.8)
[n2 (λ) + n1 (λ)]2

Here n1 (λ) and n2 (λ) are the refractive indices of the two media and both are functions of wavelength (see
Fig. 14.8). Notice the reflectance is the same no matter from which medium the light is incident on the
interface. The light not reflected is transmitted so the transmittance into the window is T12 = 1 − R12 .

5 The
sterance of a surface is the light-power emission rate per unit surface area per steradian and typically has units of W
cm−2 sr−1 .
Sec. 14.1. Photomultiplier Tubes 573

Figure 14.8. The index of refraction of a few PMT window materials as a


function of wavelength. From [Polyanskiy, 2014].

As light passes from the scintillator (medium 1) through the window (medium 2) into the PMT (medium
3), it is reflected at the two surfaces of the window. If there is no absorption of light as it passes through
the window, the minimum resulting transmittance Tmin is
" #" #
[n2 (λ) − n1 (λ)]2 [n3 (λ) − n2 (λ)]2
Tmin = [1−R12 (λ)][1−R23 (λ)] = 1 − 1−
[n2 (λ) + n1 (λ)]2 [n3 (λ) + n2 (λ)]2

16n1 (λ)n3 (λ)n22 (λ)


= , (14.9)
[n2 (λ) + n1 (λ)]2 [n3 (λ) + n2 (λ)]2
where n3 (λ) is the index of refraction of the medium light enters upon passing through the window (pre-
sumably a vacuum).
If one assumes medium 1 is air and medium 3 is a vacuum, then n1  n3 = 1, and Eqs. (14.8) and (14.9)
reduce to
[n(λ) − 1]2 16n2 (λ)
R(λ) = and T min  , (14.10)
[n(λ) + 1]2 [1 + n(λ)]4
where n is the window refraction index.
Actually, slightly more light is transmitted to the PMT than described by Eq. (14.10). Light reflected
at the PMT/window surface can be reflected at the other surface and some of this light is then transmitted
into the PMT after making three crossings in the window. Similarly, light can be reflected many times inside
the window and eventually be transmitted to the PMT. Hence the total transmittance is
(1 − R(λ))2
T (λ) = [(1 − R(λ))2 ][1 + R2 (λ) + R4 (λ) + . . .] = . (14.11)
1 − R2 (λ)
With absorption losses, light transmission through the PMT window can be approximated by
φ = τ (λ)φ0 e−α(λ)x , (14.12)
574 Light Collection Devices Chap. 14

Figure 14.9. Transmission of light through various PMT windows, each 1 mm thick,
as a function of wavelength. Corning borosilicate glasses 7740 (Pyrex), 7056, 9823, 9741
and Schott borosilicate glasses 8245 and 8250 have been usually used for PMT windows.
Schott 8337B and Heraeus Suprasil (fused quartz) are often used for extended UV PMTs.
Data are from Engstrom [1980], Donati [2000], and Schott [2014].

where φ is the transmitted flux of light, φ0 is the initial photon flux impinging perpendicular upon the surface,
x is the glass thickness, and α(λ) is the wavelength-dependent attenuation coefficient. The reflectance R(λ)
is between 0.035 to 0.05 for most glasses for which the index of refraction n  1.5. The coefficient of reflective
losses generally increases with increasing values of n.
For most scintillator detector applications, a window of borosilicate glass has a sufficiently low cutoff
wavelength that adequately allows the transmission of scintillation photons. For instance, Pyrex (Corning
7740) efficiently transmits light with wavelengths above 350 nm (see Fig. 14.9). Common borosilicate glasses
used for PMTs include Corning 7056, Corning 7740, Schott 8245, and Schott 8250. In high radiation
fields, radiation damage to the glass can cause its clarity to change, slowly becoming brownish over time.
PMTs with non-browning glass, such as Corning 9025, can be used in high radiation environments. The
transmittance of a few materials used for PMT windows are shown in Fig. 14.9. In some applications,
deeper UV emissions from a scintillator are of interest, but are attenuated by common borosilicate glasses.
For deeper UV transmission, special PMT borosilicate windows with extended UV range are used, including
Corning 9741, Corning 9823, and Schott 8337B glasses. Quartz and fused quartz (Suprasil) have excellent
deep UV transmission properties and allow the passage of photons with wavelengths down to 160 nm.
Further, the index of refraction is near 1.55, thereby producing minimal reflection losses. Because of their
extended UV range, PMTs with fused quartz windows can be used as C̆erenkov radiation detectors. Sapphire
(Al2 O3 ) windows also allow the transmittance of deep UV photons, but Al2 O3 has a high index of refraction
compared to that of glass and, thus, causes higher reflection losses, i.e., a higher R(λ), especially at lower
wavelengths.
Sec. 14.1. Photomultiplier Tubes 575

For deep UV transmission, PMTs with either LiF or MgF2 windows can be used. PMT windows man-
ufactured from LiF windows transmit photons with wavelengths down to 105 nm, below which there is
no transmittance. However, attenuation becomes significant below 120 nm, which has approximately 40%
transmittance. LiF windows are fragile and expensive to produce; hence they are used only in special appli-
cations. LiF is also slightly hygroscopic, increasing so as the temperature increases, especially above 400◦ C.6
Hence, precautions against moisture must be implemented. MgF2 is not as fragile as LiF, and is perhaps a
more popular solution for deep UV photon detection. This material allows transmission of UV photons with
wavelengths down to 125 nm before significant attenuation losses occur. The cutoff wavelength for MgF2 is
about 115 nm. Finally, PMTs without windows must be used for the detection of UV light with wavelengths
λ less than 105 nm.
Some PMT manufacturers emphasize the use of low background windows. For most applications, such a
feature is probably unnecessary. However, for low background radiation measurements, contamination from
40
K, 238 U, or 232 Th may be an issue. Borosilicate glass often has considerable contamination from these
radioactive elements, particularly from 40 K. Purified forms of borosilicate glass or fused silica (quartz), while
more expensive, are offered as low background PMT windows.

14.1.3 Photocathode Materials and Design


The main function of a PMT is to convert photons into electrical charges. This conversion is accomplished
by using the photoelectric effect, in which scintillation photons photoelectrically interact in a material coated
onto a cathode in the PMT resulting in the ejection of a photoelectron.
Quantum Efficiency, ηpc
For PMT photocathodes, the quantum efficiency ηpc is defined as the number of electrons released from the
photocathode per photon incident on the cathode,7 and is usually defined at a specific photon wavelength.
The quantum efficiency is affected by at least three different physical attributes of the absorber material,
namely the absorption efficiency, the electron diffusion length, and the energy barrier.
Absorption efficiency can be affected by the glass enclosure, the type of photocathode, and, of course,
the photocathode material. As just discussed in the section on window reflection and transmission, there
are reflected and transmitted components of the light incident on the window. The size of these components
generally depends on the wavelength of the light. Losses from reflection are generally near 8% when consid-
ering reflection on the inner and outer glass surfaces. Transmission is a function of wavelength, dropping to
only 10% transmission at the cut-off wavelength. Hence, the ηpc can be severely reduced at photon wave-
lengths approaching the cut-off wavelength of the window. The absorption efficiency of the photocathode
depends of the thickness of the material coating the photocathode. For semi-transparent (or transmission)
photocathodes, a thin layer of photosensitive material is coated upon the inner portion of the glass window,
usually only a few nanometers thick. An alternate design, less common for use with radiation detectors, is
the internal opaque photocathode, which is not coupled to the PMT window, but rather is set apart inside
the structure.
Photon absorption is restricted to those wavelengths with sufficient energy to elevate electrons into
higher electronic energy levels. For instance, if a photon has sufficient energy to elevate an electron from
the band of valence electrons into the band of conduction electrons, then the photon can be absorbed.

6 Many manufacturers of LiF optics warn against using the material above 400◦ C due to being attacked by atmospheric moisture.
7 The term quantum efficiency has several alternative definitions. It is also used to define the fraction ηλ of excited charge
carriers that radiatively recombine to release photons, a definition generally used for photon emitting devices such as LEDs
and laser diodes. For semiconductor photon detectors, quantum efficiency is also defined as the number of electron-hole pairs
produced per unit photon energy at λ. In an attempt to remedy this confusion, the authors distinguish among the various
definitions with an appropriate subscript.
576 Light Collection Devices Chap. 14

Table 14.2. Properties of a few common photocathodes. Data are from Flyckt and Marmonier
[2002] and Engstrom [1980].
Emission Radiant
λmax %ηpc
Photocathode Composition Window threshold sensitivity
(nm) at λmax
(nm) (mA/W)
S-1 AgOCs BS, SL 1100 800 2.3 0.4
S-4 SbCs3 BS, SL, FS, O 680 380 38 12
S-5 SbCs3 UV, O 630 400 50 18
S-11 SbCs3 BS, SL 700 440 80 22
S-13 SbCs3 FS 700 440 80 22
S-20 SbNa2 KCs BS, SL, FS 850 420 70 20
S-20R (ERMA) SbNa2 KCs BS, SL 900 550 35 8
S-24 SbCs3 BS 640 380 50 16
bialkali SbKCs BS, SL, FS 630 400 90 28
bialkali (GEBA) SbKCs BS, SL 630 400 90 28
bialkali (HT) SbNaCs BS, SL 700 400 50 16
solar blind CsTe FS 340 235 20 10
NEA GaAs:Cs-O UV 860 800 80 12
BS: borosilicate glass SL: soda lime glass
FS: fused silica O: opaque (reflective) photocathode
UV: Corning 9741 (UV transmitting) ERMA: extended red multialkali
GEBA: green extended bialkali HT: high temperature, data for 130◦ C

Note that absorption of such a photon may still fail to give the electron sufficient energy to escape the
conversion material. For most metals, electrons must absorb enough energy to surmount an energy barrier
at the vacuum interface of the photocathode in order to enter the vacuum of the PMT. Semiconductors, by
contrast, have relatively few electrons in the conduction band; hence electrons are generally excited from
lower energy bands (such as the valence band), and must have sufficient energy to surmount both the energy
gap between the bands plus energy to surmount the energy barrier at the vacuum interface. Long wavelength
photons may fail to transfer the required energy to surmount the vacuum barrier and, thus, generally defines
the long wavelength cut-off for many photocathodes.
Photoelectrons created very near the vacuum interface need diffuse only a short distance to the interface
where, if they have an energy above the energy barrier, they escape into the PMT. However, electrons
may diffuse in any random direction; hence, some electrons created very near the interface may diffuse in
directions away from the vacuum interface. Also, electrons produced deeper in the photocathode material
must diffuse greater distances to reach the vacuum interface, during which migration they lose energy from
collisions with ambient electrons. If these electrons reach the vacuum interface, but no longer have sufficient
energy to surmount the barrier, they de-excite to lower energy levels and can no longer escape into the
vacuum and contribute to the PMT photocurrent. All of these processes tend to reduce the overall quantum
efficiency of the photocathode. Listed in Table 14.2 are properties of a few common photocathode materials.

Work Function, φm
Photoemission is the process in which the absorption of photons in some material results in the ejection of
energetic electrons from the material. Most PMTs use metals with low ionization energies as the photocath-
odes, although many PMTs also use special semiconducting materials.
To understand the photoemission process, consider the energy level diagrams shown in Fig. 14.10. In
Fig. 14.10(a) an interface between a metal and vacuum is depicted based on the Sommerfeld model [Dekker
1957]. For an electron to escape from the metal into the vacuum, it must gain enough energy to reach the
vacuum level, E0 . The energy difference between electrons at rest in the metal and electrons at rest in the
Sec. 14.1. Photomultiplier Tubes 577

vacuum level vacuum level


E0 E0

fm
semiconductor cA
metal fm
ES
ES
EC
Eg EF
EF
EV

(a) (b)
Figure 14.10. Simplified (a) band diagram of a metal based on the Sommer-
feld model, and (b) a band diagram of a semiconductor/vacuum interface.

vacuum is denoted as ES . The Fermi energy level EF is defined as the energy below which all states are filled
and above which all states are empty at absolute zero (0 K). The minimum energy required for electrons to
move from the metal to the vacuum level is ES − EF , and is referred to as the metal work function, φm .
The energy required to move an electron at rest in the metal to the vacuum level is referred to as the outer
work function and equals ES .
The probability that an electron occupies a state with energy E is given by the Fermi-Dirac distribution
function of Eq. (12.118), repeated here for convenience,

1
fF D (E) = ,
E − EF
1 + exp
kT

where k is the Boltzmann constant, T is the absolute temperature, and EF is the Fermi energy. At absolute
zero, the Fermi-Dirac distribution function is a step function, i.e.,
$
1 E ≤ EF
fF D (E) = . (14.13)
0 E > EF

As the temperature increases, thermal energy allows some electrons to exceed the Fermi energy, provided
that energy states are available.
With the method described in Sec. 12.5.3, the density of available states about differential energy dE in
a metal is found to be (see Eq. (12.115))
√ 3/2
2me 4π(2me )3/2 1/2
N (E)dE = = E dE, (14.14)
π 
2 2 h3
or √  3/2
E 2me
N (E)dE = dE, (14.15)
2π 2 2
where h is the Plank constant and me is the electron rest mass. The product of N (E) and F (E) yields the
filled state density as a function of energy and temperature, as shown in Fig. 14.11. The total number of
578 Light Collection Devices Chap. 14

Table 14.3. Valence, Fermi energy, and work function for


metals often used in PMTs.
Fermi Energy Work function
Metal Valence
EF (eV) φm (eV)
Li 1 4.72 2.9
Na 1 3.23 2.36
K 1 2.12 2.29
Rb 1 1.85 2.26
Cs 1 1.58 2.14
Cu 1 7.07 4.45
Ag 1 5.5 4.46
Ba 2 3.8 2.51
Al 3 11.7 4.20

filled states (electrons) per unit volume can be determined by integrating the product N (E)F (E) over all
possible energies,
 ∞ 
4π(2me )3/2 ∞
n= N (E)fF D (E)dE = fF D (E)E 1/2 dE. (14.16)
0 h3 0

At absolute zero, Eq. (14.16) simplifies to


  3/2
4π(2me )3/2 EF √ π 2me EF
cm−3 .
3/2
n= E dE = = 4.55 × 1021 EF (14.17)
h3 0 3 h2

If the inner wall of the PMT tube is coated with an electron emissive material, electrons are more readily
emitted by incident low-energy photons by using a material with a relatively low work function. Inspection
of Fig. 14.12 reveals that the best candidates for photocathodes are the alkali metal elements, or mixtures
thereof. Values of the Fermi energy and the work functions for these elements are given in Table 14.3. The
overall spectral response to various photon wavelengths for the alkali metals is shown in Fig. 14.13. Some
alkali earth elements (Group II in the Periodic Table) also have low work functions, and are sometimes used
in PMTs as electron emissive materials.
Thermionic Emission
At a temperature of absolute zero, the Fermi-Dirac distribution indicates that all free electrons require
an energy equal to the work function φm to surmount an energy barrier and escape into “vacuum” (see
Fig. 14.11). As the temperature is increased, the probability that electrons are in states above the Fermi
energy EF increases. Such electrons require less energy than the work function to escape to the vacuum
level. The process whereby thermal energy in the material leads to the liberation of electrons is referred to
as thermionic emission.
The general expression for thermionic emission current density is described by the Richardson-Dushman
equation
J = A(1 − αr )T 2 e−φm /kT , (14.18)
where T is the absolute temperature, αr is a reflection coefficient that quantifies the quantum mechanical
reflection of the electron wave function at the barrier interface. The quantity A(1 − αr ) is generally referred
to as the “effective Richardson constant.” It is this thermionic emission that contributes most to the thermal
noise, or “dark current,” of the PMT device. As described by Eq. (14.18), the dark current increases as φm
decreases. However, at room temperature it turns out that the thermionic current is small and usually of
Sec. 14.1. Photomultiplier Tubes 579

Figure 14.11. The density of filled states for potassium at absolute


zero, 300 K, and 1000 K as a function of energy according to the free
electron model.

Figure 14.12. Work functions of most elements. Data are from Halas and
Durakiewicz [1998].
580 Light Collection Devices Chap. 14

Figure 14.13. Measured relative spectral response for the alkali metals. Data are from
Seiler [1920].

little consequence. With careful attention to the selection of the photocathode material, the production of
ultra-low-noise PMTs is possible.
Photoemission
Photons interacting in a photocathode material can be absorbed by free electrons. If the photon energy is
greater than the work function (hν > φm ), then electrons can be elevated to energies above the potential
barrier, and are sometimes referred to as “hot electrons.” If the electrons are excited from the Fermi energy
EF , then the resulting electron energy is simply

Ee = hν − φm . (14.19)

However, for electrons excited from deeper in the energy band, the electron energy is less, namely,

Ee = hν − (φm + E  ). (14.20)

where E  is the additional energy required for the electron to reach the vacuum level. The probability that
an electron is excited to the vacuum level from lower energy levels diminishes as E  increases. In order to
actually escape the material, these excited electrons must first diffuse to the metal/vacuum interface and
then still retain enough energy to surmount the barrier. Hence, it is less probable for electrons excited deep
in the energy band to escape as they lose energy, through scattering from ambient electrons, as they diffuse
to the boundary. Further, the deeper in the photocathode material that an electron interacts with a photon,
the less likely it is to reach the surface with sufficient energy to escape, because of the longer diffusion path
length it must travel and the increased number of energy loss interactions it undergoes as it diffuses. Hence,
a combination of diffusion effects and energy losses produce a low energy tail in the photoelectron response
distribution, as shown in Fig. 14.14.
The photocathode work function and the wavelength of photons impinging upon the photocathode gen-
erally determine the electron cutoff energy for a PMT. Photons that do not have adequate energy to excite
Sec. 14.1. Photomultiplier Tubes 581

Figure 14.14. Normalized electron response for K for two light wavelengths,
435 nm and 365 nm. Data are from Brady [1934].

electrons above the potential barrier cannot produce photoexcition. Under ideal circumstances, such a cut-
off should be represented by a step function. However, the high energy tail of the Fermi-Dirac distribution
function indicates that some free electrons in the material occupy states that exceed the Fermi energy. Con-
sequently, for photons of any given wavelength with hν ≥ φm , there are some electrons emitted with energies
greater than hν − φm , as is shown in Fig. 14.14.
Electron Affinity χA
Certain compounds of alkali metals form narrow gap semiconductors. These materials offer extended sensi-
tivity for electron excitation, but, consequently, do not follow the Sommerfeld band model. Unlike a pure
metal, electrons cannot freely flow between the valence and conduction bands, but must instead surmount
an energy gap Eg , or the band gap, between the upper edge of the valence band and the lower edge of the
conduction band. Shown in Fig. 14.10(b) is an energy band diagram for a semiconductor surface terminated
at the vacuum level. The work function of the semiconductor is still defined as the difference between the
vacuum energy level and the Fermi energy level.8 However, the Fermi energy EF is determined by the
concentration and type of dopants introduced into the semiconductor. If the concentration of negative-type,
or n-type, dopants (ND ) is greater that the concentration of positive-type, or p-type, dopants (NA ), then the
Fermi energy level moves towards the conduction band edge energy EC . Consequently, the work function
decreases. If instead the concentration of p-type dopants is greater than the concentration of n-type dopants,
then the Fermi energy level moves towards the edge energy of the valence band EV , thereby causing the
work function to increase.
Overall, both the Fermi energy level and the work function in a semiconductor are not constant, but
instead are variable depending on the doping concentration. Consequently, the work function is difficult
to use when calculating electron emission and escape probabilities. However, the electron affinity can be

8 The physics of semiconductor devices is covered in Chapter 15. However, it is important to introduce some of these concepts
here to further the understanding of a negative electron affinity photocathode.
582 Light Collection Devices Chap. 14

Table 14.4. Properties of a few semiconductor photocathode materials.

Electron Threshold Threshold


Band gap
Material affinity energy wavelength Reference
Eg (eV)
χ(E) (eV) ET (eV) λT (nm)
Na3 Sb 1.1 2.1 3.2 388 Madelung et al. 1998
K3 Sb 1.1 1.5 2.6 477 Madelung et al. 1998
Rb3 Sb 1.0 1.2 2.2 564 Madelung et al. 1998
Cs3 Sb 1.6 0.45 2.05 605 Madelung et al. 1998
Na2 KSb 1.0 1.0 2.0 620 Madelung et al. 1998
Na2 KSb:Cs 1.0 0.55 1.55 800 Madelung et al. 1998
K2 CsSb 1.0 1.1 1.88 660 Sommer 1968
K2 CsSb:O 1.0 <1.10 1.59 780 Sommer 1968
Si 1.12 4.05 5.17 240 Sze 1981
Ge 0.66 4.0 4.66 266 Sze 1981
GaAs 1.42 4.07 5.49 225 Sze 1981
p+ -GaAs 1.42 −0.02 1.4 886 Donati 2000
Gax In1−x As:Cs 1.1 0 1.1 1127 Donati 2000
p-Cs2 Te 3.2 0.2 3.4 365 Kong et al. 1995
p-InGaAsP/p-InP <1.35/1.35 <0 0.886 1400 Niigaki et al. 1997
p-InGaAs/p-InP <1.35/1.35 <0 0.729 1700 Hamamatsu 2007

treated as a constant value, defined as


χA = E0 − EC , (14.21)
where E0 is the vacuum level energy. To calculate the energy barrier heights for semiconductors, it is the
electron affinity that is typically used as a reference energy relative to the vacuum level. Hence, the photon
energy generally required to excite an electron over the vacuum barrier is

hν > Eg + χA = ET , (14.22)

where ET is the threshold energy. Note that there is a considerable concentration of electrons in the
conduction band that can be excited above the vacuum level, thereby allowing some electrons to be excited
over the barrier with an energy of only χA . However, the concentration of these conduction band electrons
is orders of magnitude below the concentration of electrons in the valence band, and, consequently, most of
the excited charge comes from electrons elevated from the valence band.
Finally, it should be mentioned that not all photocathodes are constructed from alkali metals or metal
compounds. Some photocathodes are constructed from more traditional semiconductors, such as p-type
GaAs and p-type Cs2 Te. Listed in Table 14.4 are properties of a few semiconductors used as photocathodes,
and shown in Fig. 14.15 are the absolute responsivities for many common photocathodes.9
Negative Electron Affinity −χA
To construct some photocathodes, certain doped semiconductors are used. These semiconductors form no
energy barrier at the vacuum interface! To understand the physics that cause this phenomenon, it is recom-
mended that the reader study Fig. 14.16.
Most semiconductors have a number of unbounded states on the surface. These states fill with electrons
up to a particular energy level, namely that of Fermi energy. In other words, the Fermi energy becomes

9 Theabsolute responsivity, or radiant sensitivity, is defined as the photoelectric current generated by the photocathode divided
by the number of incident photons, usually in units of mA/watt.
Sec. 14.1. Photomultiplier Tubes 583

Figure 14.15. Response functions for several photocathode materials. The


window material is soda-lime glass most of the responses. However, the S-24
response is for a 7056 borosilicate window, the CsI response is for a MgF2
window, and the Cs2 Te responses are with either a MgF2 or quartz window as
marked. Data are from Engstrom [1980] and Hamamatsu [2007].

conduction
vacuum level E0 band edge
-cA vacuum level E0
cA
conduction band edge fm cA
Eg fm
EF
Eg + cA Eg + cA
Ep EF
Eg
filled valence Ep
surface band edge
states filled
surface
valence band edge states

(a) (b)
Figure 14.16. Semiconductor band diagrams for a surface pinned to a surface state energy Ep ,
showing (a) n-type material and (b) p+ -type material with negative electron affinities.

pinned at the energy Ep , below which states are filled and above which states are empty. Note, these energy
states exist in the band gap at the surface as a consequence of unbound surface states, a condition that
generally does not exist in the semiconductor material far from the interface.
The quantity ND , used for n-type dopants, is an atomic density of impurity atoms that donate electrons to
the conduction band, thereby increasing the density of negative charge carriers (electrons) in the conduction
band. The quantity NA , used for p-type dopants, is the atomic density of impurity atoms that accept
electrons from the valence band, thereby removing electrons from the valence band and increasing the
density of positive charge carriers (holes) in the valence band.
584 Light Collection Devices Chap. 14

p-InP
substrate p-InGaAsP p-InP

p-InP
substrate p-InGaAsP p-InP conduction band
vacuum
Eb level
conduction band Eg = 1.35 eV vacuum level

EF
Eg = 1.35 eV

valence photon
EF E0 band absorption applied voltage
layer bias (+)

valence photon
band absorption electron electron
layer emission emission
layer electrode layer
electrode

(a) (b)
Figure 14.17. Semiconductor band diagrams for a field-assisted InP/InGaAsP/InP heterostructure pho-
tocathode (a) under zero bias and (b) under reverse bias operation.

By strongly doping a p-type semiconductor, the Fermi energy level in the bulk semiconductor is lowered
close to EV as shown in Fig. 14.16(b). At equilibrium, the Fermi energy must be constant across the interface
and, hence, the energy bands bend accordingly to satisfy this condition such that the Fermi energy level in
the bulk aligns with the pinned Fermi energy level at the surface. Consequently, the vacuum level E0 at
the surface moves below EC in the bulk semiconductor, producing a negative electron affinity as calculated
from Eq. (14.21). As a result, electrons can now move from the semiconductor bulk at energy EC into the
vacuum without encountering an energy barrier [Rougeot and Baud 1979].
Heterostructure negative electron affinity (NEA) photocathodes take advantage of semiconductor band-
gap engineering to extend the IR response of PMTs while maintaining relatively high sensitivity. The
structures are fabricated by growing an epitaxial p-type InP layer upon a p-type InGaAs or InGaAsP layer,
as depicted in Fig. 14.17. The InP semiconductor layer has a much wider band-gap than the InGaAs (or
InGaAsP) layer [Niigaki et al. 1997]. Because these epitaxial crystals are thin, typically with thicknesses of
0.2 to 0.5 μm, it is usual to grow them upon relatively thick InP substrates so they are forced to function as
opaque (reflection) type photocathodes. Front windows with InP-based semi-transparent type heterostruc-
ture semiconductor photocathodes are also manufactured, but because of their poor absorption of photons
above 1.35 eV, they suffer reduced sensitivity for photon wavelengths below 900 nm. The surface of the
p-type InP layer forms a NEA boundary at the vacuum boundary, but there is still a barrier to surmount
at the InGaAs/InP (or InGaAsP/InP) interface, as shown in Fig. 14.16(a). Application of a bias voltage
to the photocathode lowers the conduction band barrier, thereby allowing electrons to more easily to pass
into the vacuum, as shown in Fig. 14.16(b). These NEA photocathodes have sensitivity at photon wave-
lengths extending up to 1400 nm for the InGaAsP/InP type and up to 1700 nm for the InGaAs/InP type
[Hamamatsu, 2007]. Advanced heterostructure photocathodes can operate up to 2300 nm [Niigaki et al.
2014]. Unfortunately, heterostructure semiconductor photocathodes also have a high dark current when
used at room temperature; hence they must be cooled to temperatures between −60◦ C and −80◦ C during
operation.
NEA photocathodes enable electrons to diffuse greater distances before dropping back to the conduction
band edge and recombining with holes. This greater diffusion distance allows thicker photocathodes to
Sec. 14.1. Photomultiplier Tubes 585

Figure 14.18. Response functions for several photocathode materials that are usu-
ally used for detection of longer wavelength light. Data are from Engstrom [1980] and
Hamamatsu [2007].

be used while improving the electron emission. Hence, NEA photocathodes can have much higher photon
response than common alkali metal photocathodes, especially in the long wavelength region, as can be seen
from Fig. 14.18.

Semi-Transparent and Opaque Photocathodes


Photocathodes are either applied directly to the inner surface of the entrance window to the PMT enclosure
or upon an internal secondary surface within the enclosure. Photocathodes applied to the inner surface of
the transparent envelope are designed with thicknesses on the order of only a few electron diffusions lengths
(tens of nanometers) and, therefore, are semi-transparent. Internal photocathodes are set back from the
entrance window do not suffer the same problem and can have thicker material layers laid upon a substantial
conductive backing, and are, therefore generally opaque. There are advantages and disadvantages to both of
these designs.
Semi-transparent photocathodes are deposited upon the inside surface of the PMT entrance window, a
geometry that enables the scintillation material to be placed adjacent to the photosensitive material. This
usual arrangement serves to increase the solid angle between the light source and photosensitive area, thereby
maximizing the detector signal. Such an arrangement is depicted in Fig. 14.2 and shown in Fig. 14.3. Because
photoelectrons are ejected into vacuum from the side of the photocathode material opposite that upon which
light is incident, this type of photocathode is sometimes called a transmission photocathode.
The thickness of a semi-transparent photocathode must be carefully controlled. If the photocathode is
too thick, then photons can be absorbed beyond the critical escape depth for photoelectrons. Hence, any
additional material serves only to decrease the electron signal. If the photocathode is too thin, then many
of the incident photons pass through the photocathode without producing photoelectrons.
For opaque photocathodes, electrons are ejected from the same side as that upon which the light is
incident. These photocathodes are often called reflective photocathodes. In these photocathodes the self-
586 Light Collection Devices Chap. 14

absorption of photoelectrons is no longer a limiting factor, and opaque photocathodes can be applied as
thicker layers. However, because they are set back from the PMT entrance window, opaque photocathodes
may suffer loss of light because of a decreased solid angle with respect to the light source.
Optical power transmission through the photocathode material is described by

P (x) = P (0)e−α(λ)x , (14.23)

where α(λ) is the attenuation coefficient at a specific wavelength λ and x is the distance from the cathode
surface along the direction of light travel. The inverse of α(λ) is the attenuation length in which a fraction 1−
e−1  63% of the incident photons are absorbed. Optical power absorption is greatest at the vacuum interface
for opaque photocathodes, whereas it is least at the vacuum interface for semi-transparent photocathodes.
If one assumes that the number of photoelectrons is proportional to the profile of absorbed light energy, the
distribution of electron-hole pairs created in the photocathode is

Fe (x) = ke α(λ)P (0)e−α(λ)x dx, (14.24)

where ke is a constant. Once a photon has been absorbed, and presumably produced an excited electron-
hole pair, photoemission from the photocathode occurs only if (a) the photoelectron energy is greater than
the threshold energy ET = Eg + χA , and (b) the photoelectron can diffuse to the vacuum boundary while
retaining E ≥ ET .
It is possible for an electron to become excited from photon absorption but with an energy hν < ET .
However, the photoelectron does not have sufficient energy to surmount the energy barrier depicted in
Fig. 14.10 and, consequently, cannot reach the vacuum. The threshold wavelength is defined as
hc 1239.8
λT = = {nm}, (14.25)
Eg + χA ET
where ET is expressed in eV. The threshold wavelength for many photocathode materials are listed in Table
14.4.
The photoelectrons must also be able to diffuse to the vacuum boundary while maintaining sufficient
energy to surmount the energy barrier. Although the threshold energy ET is the theoretical minimum
energy limit, photoelectrons actually require much more initial energy than ET to escape the photocathode
in order to compensate for energy losses experienced during their diffusion to the interface. Because the
electrons diffuse in random directions, many photoelectrons diffuse away from the vacuum boundary. Also,
as the photoelectrons diffuse through the photocathode material, they lose substantial energy with each
scatter reaction. A scatter can also cause the electrons to radically change directions. Each scatter may
result in the energy of an electron dropping below ET or change direction so it diffuses away from the vacuum
boundary, either case negating photoemission. Overall, for a wide spectral response, the initial energy Epe
of the photoelectron should be greater than the threshold energy, i.e.,
hc
= Epe ET . (14.26)
λ
14.1.4 Dynode Materials
Energetic electrons, such as accelerated photoelectrons, impinging onto a surface can cause the emission of
secondary electrons, provided that the energy transferred to secondary electrons is greater than the vacuum
barrier. The secondary electron yield δ is defined as
Ns
δ= , (14.27)
Np
Sec. 14.1. Photomultiplier Tubes 587

where Ns is the number of emitted secondary electrons and Np is the initial number of primary electrons
striking the material.
There are similarities between photoemission and secondary electron emission, the distinctive difference
being that photoelectrons are a result of the photoelectric effect and secondary electrons are created through
coulombic interactions between the incident primary electron and the ambient electrons of the material.
Because a single primary electron can scatter from many secondary electrons in the material, there is a
possibility that many electrons acquire enough energy to surpass the vacuum barrier. Some of the energetic
secondary electrons may, in turn, interact with other electrons transferring sufficient energy to allow them
to also escape. Thus, if the primary electron has sufficient initial energy, the gain of Eq. (14.27), is greater
than unity.
Typically photoelectrons emerging from the photocathode surface do not have sufficient energy to produce
secondary electron emission. However, this situation is easily remedied by applying a secondary electron
emission material upon an electrode, referred to as a dynode, and applying an accelerating voltage to it. The
photoelectron can then gain sufficient kinetic energy as it is attracted to the anode to promote secondary
electron emission.
Secondary Electron Emission
As with photoelectron emission, a series of processes must take place for successful secondary electron
emission. These processes include, (a) the primary electron acquiring an energy greater than ET of the
dynode material, (b) the excited secondary electrons then must diffuse in the direction of the vacuum barrier,
and (c) the secondary electrons, upon reaching the vacuum barrier, must still retain an energy greater than
ET .
As the energy of the primary electron is increased, the maximum depth of secondary electron genera-
tion also increases. Consequently, secondary electrons generated deep in the dynode material must diffuse
relatively long distances to reach the vacuum boundary compared to those secondary electrons generated
near the surface. If the primary electron is normally incident on the dynode, the maximum depth a primary
electron can reach in the dynode material is the continuous-slowing-down-approximation range RCSDA dis-
cussed earlier in Sec. 4.6.3. To reach this maximum depth the electron trajectory must be almost a straight
line, i.e., no large angle scatters. However, very few of the incident electrons produce such trajectories and
reach such depths. Of more utility is the mean forward or projected range Rp defined as the expected or
average maximum depth of penetration in the direction of the incident electron. However, the calculation
of Rp from first principles requires detailed electron transport calculations that take into account quantum
mechanical and electron binding effects in the ambient atoms. Alternatively, the CSDA range RCSDA can be
multiplied by the appropriate detour factor to give Rp . But tabulations of detour factors are hard to find and
their calculation also requires extensive electron transport calculations. Because primary photons generated
in a PMT seldom have energies above a few keV, it is better to base range calculations on experimentally
determined ranges.
Young [1956] experimentally determined the primary electron penetration mass thickness in Al2 O3 is
described by
ρR = 0.0115Eo1.35, (14.28)
where Eo is in keV and ρR is in units of mg cm−2 . From Fig. 4.23 it is seen that the mass-thickness range
for any given monoenergetic electron is nearly the same for a wide range of materials ranging from air to
gold. Thus, the penetration range for all dynode materials can be estimated by
1.15 × 10−5 1.35
R Eo , (14.29)
ρ
where R is in cm, ρ is the dynode material density (g cm−3 ) and Eo is in units of keV.
588 Light Collection Devices Chap. 14

Example 14.2: Calculate the electron range as a function of energy for Al2 O3 , MgO, BeO, and GaP for
accelerating voltages between 0 to 5 keV.

Solution:
The densities of Al2 O3 , MgO, BeO, and GaP are 3.99, 3.58, 3.01, and 4.14 g cm−3 , respectively. From
Eq. (14.29), the penetration depth for Al2 O3 is,

1.15 × 10−5 1.35


R E ,
3.99 g cm−3 o
yielding the results depicted in Fig. 14.19. The ranges for the other materials are found in the same manner.
These results indicate that, for accelerating voltages less than 1000 volts, the penetration depth R is limited
to less than 50 nm for these materials.

Figure 14.19. Calculated penetration depths for Al2 O3 ,


MgO, BeO, and GaP as a function of primary electron energy.

Models for Secondary Electron Emission


The secondary electron emission yield δ, defined as the ratio of emerging secondary electrons to impinging
primary electrons, can be described by [Dekker 1958]

δ = n(x, Eo )fesc (x)dx. (14.30)

Here n(x, Eo )dx is the number of secondary electrons produced at depths in dx about x by a primary electron
of initial energy Eo , and fesc (x) is the probability that a secondary electron produced at depth x reaches
the vacuum interface and is emitted or escapes. The escape probability of secondary electrons, to a first
approximation, may seem to be a simple solid angle problem defined by the diffusion length and excitation
distance from the surface. However, the complex nature of electron scattering and transport causes the
probability of emergence to be somewhat complicated [Simon and Williams, 1968].
Sec. 14.1. Photomultiplier Tubes 589

Table 14.5. Maximum yields δom of secondary electrons and optimum initial energy Eom
of the incident primary electron for some elements. From Dekker [1958].
Eom Eom Eom
Material δm Material δm Material δm
(eV) (eV) (eV)
Li 0.5 85 Be 0.5 200 B 1.2 150
Mg 0.95 300 Al 0.95 300 Si 1.1 250
K 0.7 200 Ti 0.9 280 Fe 1.3 400
Co 1.2 500 Ni 1.3 550 Cu 1.3 600
Ga 1.55 500 Ge 1.15 400 Rb 0.9 350
Zr 1.1 350 Nb 1.2 375 Mo 1.25 375
Pd >1.3 >250 Ag 1.4 800 Cd 1.1 450
Sn 1.35 500 Sb 1.3 500 Cs 0.7 400
Ba 0.8 400 Ta 1.3 600 W 1.3 650
Pt 1.8 700 Au 1.4 800 Hg 1.3 600
Tl 1.7 650 Pb 1.1 500 Bi 1.15 550

For any element the yield δ of secondary electrons varies with the energy Eo of the incident primary
electron. There is an optimum energy Eom that produces the maximum yield δm of secondary electrons for
a particular element. Some optimum yields and energies are given in Table 14.5.
There are many models describing secondary electron emission yield. For example see Dekker [1958] and
Adamson [1993]; however, only two of the more important models are described here, namely, the power law
model and the constant loss model.
Power Law Model Baroody [1950] developed a theory for secondary electron yield based on the concepts
that (1) the production of secondary electrons per unit pathlength of travel by the primary electron is
proportional to the rate of energy loss −dE/dx, and (2) these secondary electrons are exponentially absorbed
in the target material as they diffuse towards the surface. Hence, the secondary electron yield per incident
primary electron is given by
 R
dE −αx
δ = −K e dx, (14.31)
0 dx
where K is a proportionality constant and α is the electron absorption coefficient. According to Whid-
dington’s Law [Whiddington 1912], the energy loss per unit distance for the primary electron is inversely
proportional to the energy at depth x from the surface, i.e.,
dE(x) A
− = , (14.32)
dx E(x)
where A is a constant dependent on the dynode material. Rearrangement and integration yield

E(x) = Eo2 − 2Ax. (14.33)
However, according to Lye and Dekker [1957], Whiddington’s Law does not produce reliable results, and
instead they proposed that Eq. (14.32) should be modified to
dE(x) A
− = n , (14.34)
dx E (x)
where again A is a constant dependent on the material. Rearrangement and integration then gives the energy
of the primary electron at depth x as
E n+1 (x) = Eon+1 − A(n + 1)x. (14.35)
590 Light Collection Devices Chap. 14

Because E n+1 (R) = 0 setting x = R in Eq. (14.35) gives the primary electron range as
 Eo n
E Eon+1
R= dE = . (14.36)
o A A(n + 1)
Note that Eq. (14.36) with n = 0.35 agrees with the experimental result of Eq. (14.28).
With the assumption that the production of secondary electrons is proportional to −dE/dx, and that
the function fesc (x) is proportional to e−αx , then Eq. (14.31) becomes
 R
A
δ=K − n e−αx dx. (14.37)
0 E (x)
After much manipulation and change of variables, this equation can be written as
1/(n+1)
A(n + 1)
δ=K Fn (r), (14.38)
α
where the function Fn (r) is defined as
 r
(n+1) (n+1)
Fn (r) ≡ e−r ey dy, (14.39)
0

and r is defined as
αEon+1
rn+1 = αR = . (14.40)
A(n + 1)
The maximum secondary electron yield δm is found by setting dδ/dEo = 0. The result is [Lye and Dekker
1957]
1/(n+1)
A(n + 1) 1
δm = K n
, (14.41)
α (n + 1)rm
where rm is the value of r at the maximum secondary electron yield. Lye and Dekker [1957], combined
Eqs. (14.38) and (14.41) to obtain a normalized curve yield that is independent of the material properties,
namely,
δ n Fn (rm Eo /Eom )
= (n + 1)rm Fn (r) = , (14.42)
δm Fn (rm )
where Eom is the initial energy that maximizes the secondary electron yield, and Eo /Eom = 1 when δ/δm = 1.
Baroody [1950] evaluated Eq. (14.39) for n = 1 by using a series expansion to obtain
 r  ∞
2 2 (−1)i r2i+1
F1 (r) = e−r ey dy = , (14.43)
0 i=0
i!(2i + 1)

although today with our PCs Fn (r) is readily evaluated numerically. Baroody [1950] determined that F1 (r)
had a maximum value at rm = 0.92, hence,
δ F1 (0.92Eo /Eom )
= = 1.85F1 (0.92Eo /Eom ). (14.44)
δm F1 (0.92)
Baroody’s treatment followed the general trend for secondary electron yield, but had large deviations from
experimental data for Eo /Eom > 1.1, as can be seen from Fig. 14.20. Later, Lye and Dekker substituted
n = 0.35 into Eq. (14.42), based on the findings of Young [1956], to yield a power law solution that agrees
considerably better with experimental values than does Baroody’s model. A comparison of these two power
law models is shown in Fig. 14.20.
Sec. 14.1. Photomultiplier Tubes 591

Figure 14.20. Comparison values of δ/δm for experimental data and theo-
retical models. Experimental data:  Ge, •MgO,  Mo, ♦ Pt, ◦
Li; and
are taken from from Kollath [1937], Baroody [1950], Whetten and Lamponsky
[1957], Lye and Dekker [1957], Johnson and McKay [1954], and from Simon
and Williams [1968].

Constant Loss Model The secondary production rate n(x, Eo ) in Eq. (14.37), according to Eq. (14.31), is
given by
1 dE
n(x, Eo ) = − , (14.45)
w dx
where w is the average absorbed energy needed to create an ion-electron pair, and the electron escape
function fesc (x) in Eq. (14.37) is
fesc (x) = B1 B2 e−αx , (14.46)
where 1/α is the mean-free-path length of secondary electrons or, equivalently, α is the probability, per unit
differential path length of travel, a secondary electron is absorbed. B1 is the probability that an electron
diffuses in the direction of the vacuum boundary, and B2 is the probability that upon reaching the vacuum
boundary that the secondary electron still has sufficient energy to surmount the vacuum boundary, i.e., an
energy above ET . The term B1 is assumed to have the value of approximately 0.5; however, when considering
scattering and solid angle effects, B2 should be a function of the depth at which the secondary electron is
liberated. For simplicity, Simon and Williams [1968] treat B2 as a function independent of x, thereby greatly
reducing the complexity of calculating δ. For a secondary electron created at the surface x = 0, the product
B1 B2 = 0.5. If it is assumed that energy loss of the primary electron is approximately constant over the
primary electron range,10 the change in energy with travel distance can be expressed as,
dE Eo
−  . (14.47)
dx R
10 Theassumption of a constant stopping power is valid for electrons with energies above 1 MeV, but not strictly true for lower
energy electrons. In Sec. 4.6, a more rigorous treatment of electron ranges and stopping powers is presented.
592 Light Collection Devices Chap. 14

Figure 14.21. Escape probability and number of electrons liberated in MgO


as a function of primary electron energy. After Simon and Williams [1968].

Substitution of Eqs. (14.45), (14.46), and (14.47) into Eq. (14.30) yields,
 R
B1 B2 Eo −αx B1 B2 Eo : ;
δ= e dx = 1 − e−αR . (14.48)
0 w R wαR
Because it is assumed that there is a constant energy loss as the primary electron travels through the
material, the total number of excited secondary electrons is Eo /w, and the number of electrons excited, per
unit pathlength of the primary electron, is
1 dE Eo
− = . (14.49)
w dx wR
In Fig. 14.21 fesc (x) and secondary electron production are shown for MgO.
From Eq. (14.36), the primary electron range can be written as R = Cm Eon+1 where Cm is a constant,
so that Eq. (14.48) is rewritten as  
1 − e−αCm Eo
n+1

δ = Km Eo . (14.50)
−αCm Eon+1
where Km is a combination of constants. There is some value Eo at which δ reaches a maximum value δm .
This value can be found by setting dδ/dEo = 0. Again the total gain of secondary electron emission, as a
function of Eo , reaches a maximum value, beyond which δ begins to decrease.
To find a normalized dependence of δ on Eo , Lye and Dekker [1957] define a variable z ≡ αCEon+1 so,
from Eq. (14.50) it is seen that δ is proportional to the function
n+1
1 − e(−z )
fn (z) ≡ . (14.51)
zn
Hence, the general normalized dependence of δ on Eo is given by
δ fn (zm Eo /Eom )
= . (14.52)
δm fn (zm )
Sec. 14.1. Photomultiplier Tubes 593

Table 14.6. Secondary electron emission properties of some


materials. From Dekker [1958].
Density Eom 1/α w
Material δm
(g cm−3 ) (keV) (nm) (eV)
Pt 21.45 1.8 0.7 2.0 80
Ge 5.35 1.15 0.4 3.5 71.5
MgO 3.58 24 1.2 23 10.25

Figure 14.22. Secondary electron emission ratios for many materials used as
dynodes in photomultiplier tubes. After [Engstrom 1980].

A plot of Eq. (14.52) with n = 0.35 is shown in Fig. 14.20. From the results in Fig. 14.20, it is seen that
the constant loss model yields the best agreement with experiments, particularly when compared to the
power law model and Baroody’s analysis. Values of some model parameters for three materials are given in
Table 14.6.
What important lessons are learned from the above analysis? Mainly, for any given dynode material,
there is an optimum primary electron energy that yields the highest secondary electron yield. Further, the
secondary electron emission yield of most materials can be described by a universal reduced yield curve,
as shown in Fig. 14.20. The yield ratio is the number of secondary electrons emitted per incident electron.
Experimentally measured yield ratios for many dynode materials are plotted in Fig. 14.22.

14.1.5 PMT Dynode Designs and Configurations


The shape and placement of the dynodes within the PMT determine the efficiency by which electrons are
liberated and collected from each dynode stage. Calculated results can lead to efficient high-gain designs.
It is interesting to note that, before the era of the modern electronic computers, such calculations were
assisted with mechanical models, which included stretched rubber diaphragms and electrical resistor models
[Engstrom 1980]. By arranging stretched rubber diaphragms between the “electrode” stage in the model,
594 Light Collection Devices Chap. 14

Table 14.7. Properties of some common dynode designs. After Hamamatsu [2007].

Dynode Rise time Pulse linearity Collection Main


Uniformity
design response (ns) at 2% (mA) efficiency characteristic
circular cage 0.9–3.0 1–10 poor good compact and
high speed
box-and-grid 6–20 1–10 good very good high collection
efficiency
venetian blind 6–18 10–40 good poor large diameter

linear focus 0.7–3 10–250 poor good high speed


and high
linearity
mesh 1.5–5.5 300–1000 good poor high magnetic
immunity and
high linearity
metal channel 0.65–1.5 30 good good compact and
high speed
Micro-channel plate 0.1–0.3 700 good poor high speed

the height (potential energy) was adjusted to correspond to the electrical potential, and balls released upon
the platform would follow the general path expected for electrons within the PMT. Hence, a simple dynode
configuration could be designed with this tool. Electrically based models used a network of resistors in a grid
pattern. By setting those resistors corresponding to a dynode plane in the model to a uniform potential, the
electric potential between these planes could be directly measured between the electrodes.
Computer simulations of electron trajectories, voltage potentials, photocathode shape and focusing elec-
trodes, dynode shapes and materials, are now routinely used for design of modern PMTs. Electrons emitted
from the photocathode are focused onto a small area of the first dynode. Afterwards, secondary electrons
emitted from the first dynode are directed to the next dynode, and so on until they reach the anode. The
anode is specially designed to improve collection efficiency while suppressing space charge limitation effects.
Most modern PMT designs have electron collection efficiencies η approaching 100%.
Designs for the Electron Optics
There are numerous photocathode and dynode geometries employed in PMTs, a few of which are described
here. More details on these designs can be found elsewhere [Engstrom 1980; Flyckt and Marmonier 2002;
Hamamatsu 2007]. A summary of some important properties of the different geometric designs, discussed
below, is provided in Table 14.7.
Circular Cage Design The first successful commercial PMT was the 931A, developed by RCA and shown
in Fig. 14.1, which used the circular cage design. This dynode design, shown in Fig. 14.23, is relatively
compact and can be used for both the transmission or reflection type of PMTs. The original design had
an opaque photocathode, depicted in Fig. 14.23(left), which was illuminated from the side. The 931A and
931B PMTs, both 9 stage circular cage dynode devices, are relatively small with diameters of 1.125 inches.
Both provide high gains (931A  5.5 × 106 , 931B  6 × 106 ), and can be used for scintillation samples that
do not require coupling to a large photocathode. The envelope is composed of soda-lime glass. However,
the photoresponses are different, mainly because the 931A has an Cs3 Sb photocathode and the 931B has
a K2 CsSb photocathode. Typically, the 931B offers higher photocathode quantum efficiency, higher anode
sensitivity, and lower dark current than the 931A. The compact sizes ensure a rapid time response or short
Sec. 14.1. Photomultiplier Tubes 595

focusing
electrode
3 1 4
2

grill 5
6
3
4 2 7
5 9 photo-
incident electrons incident
6 radiation 8 radiation
8 0
10 1

shield anode
shield
9
7
anode

1-10: dynodes semi-transparent


0: opaque photocathode photocathode
1-9: dynodes

Figure 14.23. The circular cage dynode configuration showing (left) an opaque (reflection) photocathode
arrangement and a (right) semi-transparent (transmission) photocathode arrangement. After [Engstrom 1980].

transit time of about 18 ns for the 931 tube series. The electron transit time is defined as the time interval
between a photo-impulse impinging on the photocathode and the corresponding output pulse at the anode
terminal to reach its peak amplitude. Advanced versions of the circular cage PMT have faster response times
that range between 0.9 and 3.0 ns. A weakness in the design is the existence of a small electrostatic field
at the apex of the grill and photocathode shown in Fig. 14.23(left). This field causes poor photoelectron
collection efficiency in that region.
An alternative design of the circular cage dynode bank is shown in Fig. 14.23(right), in which the
device has a much larger primary dynode and a semi-transparent photocathode. The flat semi-transparent
photocathode allows a relatively large scintillation crystal to be directly coupled to the PMT. The design also
has a focusing electrode, which, along with the large primary dynode, improves the photoelectron collection
efficiency. Although this configuration of the PMT still has a rapid time response, the electron transit time
is lengthened compared to the traditional circular cage dynode design because of the extra time required for
electrons to traverse the distance between the photocathode and the primary dynode.

Venetian Blind Design The venetian blind design, see Fig. 14.24, offers excellent photoelectron collection
and is ideally suited for “head-on” photomultiplier tubes because of its large photocathode diameter. The
large photocathode permits good photon collection and is positioned relatively far from the first set of dynode
blades. The photoelectrons are focused with steering electrodes onto the first set of dynode blades so as to
achieve collection efficiency of nearly 100%, a feature necessary for good gamma-ray spectroscopy. Secondary
electrons emitted from the dynode surfaces are steered into the next set of dynode vanes with accelerating
grids. Consequently, some secondary electrons can be lost by collisions with these grids, thereby reducing
overall secondary electron collection efficiency (i ) between dynode stages. Further, the potentials across
the dynode paths are relatively low, thereby reducing the electron speeds and causing the transit time and
response time of the PMT to lengthen. In summary, the venetian blind design enables PMTs to be coupled
to relatively large scintillation crystals, offers high photoelectron collection efficiency, but has a relatively
slow time response. Because of the slow response, this type of PMT now has somewhat limited use.

Box and Grid Design The box and grid design (Fig. 14.25), widely used in head-on photomultiplier tubes,
has better photoelectron collection efficiency than most PMTs. This design incorporates a relatively large
entrance window and photocathode. Accordingly, photomultiplier tubes using this dynode offer high detec-
tion efficiency and good uniformity. Similar to the venetian blind design, photoelectron collection is nearly
596 Light Collection Devices Chap. 14

internal
conductive
coating semitransparent
photocathode
anode dynodes focusing
electrode

incident radiation

focusing
accelerating grids electrode
internal
conductive
coating

Figure 14.24. The venetian blind dynode configuration for a semi-transparent (trans-
mission) photocathode. After [Engstrom 1980].

7 6 3 2 incident radiation

anode box photo-


9 8 5 4 electrons
1
accelerating
grids focusing
electrode

1 - 9: dynodes

Figure 14.25. The box and grid dynode configuration for a semi-transparent
(transmission) photocathode. After [Engstrom 1980].

100%, an attribute necessary for good gamma-ray spectroscopy. Each dynode has a grid electrode at the
entrance, which assists with electron acceleration and steering. However, the weak electric fields between
dynodes reduce electron speeds and, thus, produce a relatively slow time response. Regardless, this type of
PMT still is used today as the light sensor for many scintillator/PMT detectors.

Linear Focus Design The linear focus, or in-line, dynode configuration is widely used in head-on pho-
tomultiplier tubes. Its attractive features include fast time response, good time resolution and excellent
pulse linearity. A linear focus PMT attached to a NaI:Tl crystal is shown in Fig. 14.4. The linear focus
dynode configuration is often employed with a curved photocathode as depicted in Fig. 14.26. The curved
photocathode reduces the variance in electron pathlengths, as compared to a common flat photocathode.
This smaller pathlength variance, in turn, reduces the variance in arrival time of electrons striking the first
dynode. However, a curved photocathode makes it difficult to couple the PMT to scintillation crystals. As
a consequence, linear focus dynode PMTs are also available with a flat photocathode surface. The dynodes
aligned in the linear focus arrangement also reduces the variance in the arrival time of electrons as they
eventually arrive at the anode. This compensation is accomplished with curved interposed dynodes designed
to alternate between the longer and shorter electron pathlengths moving through weaker and stronger elec-
Sec. 14.1. Photomultiplier Tubes 597

anode focusing faceplate


electrode photocathode electron
trajectories
incident 5V
radiation
dynodes 20 V

dynode 1 50
equipotential
lines
semitransparent 80
photocathode
100

125
dynode 4

dynode 2
0 0
200
400

photoelectron 550 550


dynode 5 dynode 3
600 600

dynode 1 photoelectron
dynode 1

Figure 14.26. The linear focus dynode configuration showing (left) the dynode arrangement and (right) the focused
electron trajectories from the curved photocathode. After [Engstrom 1980].

tric fields. Consequently, the total electron transit times for electrons passing through the dynode bank are
nearly equal. An electron trajectory sequence is depicted in Fig. 14.26(bottom left). Overall the electron
transit times and their variance are superior to most PMT designs.
Compact Dynode Designs A compact dynode configuration allows PMTs to be fabricated in relatively
short containers. They typically have higher resistance to magnetic field interference, but they have lower
gains. These compact PMTs are available as single channel PMTs or position sensitive PMTs. The dynodes
most often used are described below.
Mesh Dynodes The mesh dynode is composed of interspersed parallel wire planes that form a system
with the appearance of a wire screen; however, the wire planes are stacked, not interwoven. The wires
may have a triangular cross section and are coated with secondary electron emission materials, as shown in
Fig. 14.27(left). Each electrode layer is rotated 90◦ to the prior layer such that they are oriented in the x
and y directions. Multiple stacked layers are used in close proximity to form a compact dynode array that
can be used to provide x and y position information for imaging purposes. There are basically two types
of design: a coarse mesh type and a fine mesh type. Both are excellent in output linearity and have good
immunity to magnetic fields. Position sensing versions have either cross wire anodes or multianodes and
can provide the location of photon interactions upon the photocathode. However, the devices generally have
poor spatial resolution because of the spatial spread of the electron cascade, which is about 8 to 9 mm. Fine
mesh types are developed primarily for photomultiplier tubes that are used in high magnetic fields. Some
versions have magnetic immunity up to 1500 mT. The electric field and voltage drop between stages are low,
hence the gain is typically lower than that of conventional PMTs. Gains on the order of 105 or more are
achievable for systems with many stages (≥ 12).
Metal Foil Channel Metal foil channel dynodes are made with perforated foils coated with materials
that produce secondary electrons. PMTs using these dynodes have properties similar to those of venetian
blind PMTs, including the problem with electron collection. These dynodes can be used as position sensing
PMTs with resolutions better than those of PMTs using mesh dynodes. With a resistive divider circuit,
spatial resolution of approximately 4 to 5 mm can be achieved. The electric field and voltage drop between
stages are low; hence, the gain is typically lower than conventional PMTs. Because the foils can be stacked
in close proximity, metal foil channel PMTs can be fabricated in compact packages for special applications.
598 Light Collection Devices Chap. 14

photoelectrons photoelectrons

Figure 14.27. Compact photomultiplier dynode configurations, showing the


basic scheme for (left) wire mesh dynodes and (right) metal foil channel dyn-
odes.

Further, metal foil channel PMTs have higher magnetic immunity than most PMTs (up to fields of about
5 mT), except for mesh dynode PMTs. Gains on the order of 105 or more are achievable for systems with
many stages (≥ 12).

Microchannel Plates Use of microchannel plates is another method for amplifying signals from a scin-
tillator and are closely akin to the Kubetsky tube. Microchannel plates are bonded clusters of glass tubes,
each usually having a diameter between about 15 to 50 μm, whose inside is coated with materials that emit
secondary electrons as is shown in Fig. 14.28. The individual channels are referred to as “continuous channel
electron multipliers” [Wiley and Hendee 1962]. A voltage is applied across the tube length which causes
electrons to cascade down the tube. When an electron strikes the tube wall, more electrons are emitted,
much as with dynodes in a PMT. Hence, a single electron can cause a cascade that can eventually produce
more than 106 electrons that reach the other end of the tube. Typically, thousands of these continuous
channel electron multipliers are bonded together to form a PMT.
At sufficiently high gains, the pulse can also become saturated, thereby compromising the pulse height
distribution. In other words, regardless of the photon electron density striking the microchannel plate,
all output pulses have nearly the same amplitude. A study conducted by Schmidt and Hendee [1966]
indicates that space charge accumulation of electrons in the channel causes this saturation effect. Emission
of energetic electrons can also cause sputtering as they strike the walls or anode, thereby liberating positive
ions into the channel. These positive ions can travel in the opposite direction of the electrons and cause
more electron emissions as they strike the walls, a process termed as “ion feedback.” Consequently, the
pulse rise time is extended by successive waves of secondary electrons, often over ten times the expected
values. It was found that bending the continuous channel electron multipliers would remedy this feedback
problem [Evans 1965], because electrons can drift towards the anode around the bend whereas ions cannot
drift backwards before striking the wall with insufficient energy needed cause secondary electron emission.
Modern microchannel plates used in PMTs are often arranged in a chevron configuration to eliminate ion
feedback. Regardless, space charge effects can appear for gains of more than 107 and can still produce pulse
height spectra saturation.
The microchannel plate can be substituted for the staged-dynode bank inside a vacuum tube to operate
as a PMT [Chevalier et al. 1970]. Energetic photoelectrons entering can cause the ejection of secondary
electrons, which cascade down the microchannels to liberate millions more electrons. The main advantage of
a microchannel plate is its compact size. A microchannel plate only one-inch thick can produce a signal of
similar strength as a conventional staged-dynode PMT. Microchannel plates have relatively fast rise times
[Piétri 1975], typically between 100 and 300 ps, and a relatively small spread of transit times, usually less
Sec. 14.1. Photomultiplier Tubes 599

photocathode

photoelectron anode

V
photon

V
glass envelope MCP

Figure 14.28. (left) Depiction of electron multiplication in a microchannel. (right) Depiction of


a microchannel plate PMT.

than 100 ps. Further, microchannel plates have found use as image intensifiers, in which their compact and
small channels provide excellent spatial resolution. The main problem with using microchannel plates is that
the signal produced, per monoenergetic radiation event, is statistically much noisier than that produced by
a PMT. Hence, spectroscopic energy resolution is usually worse than that produced by a multistage dynode
PMT.

14.1.6 Gain
The gain G of a PMT is defined as the average total number of electrons collected at the anode Na divided
by the average total number Npc of photoelectrons initially ejected from the photocathode, i.e.,

Na qe Na Qa
G= = = , (14.53)
Npc qe Npc Qpc

where qe is the unit charge, Qpc is the average charge emitted from the photocathode and Qa is the average
charge delivered to the PMT anode. The number of collected electrons Na can be calculated from the
dynode charge collection efficiency η and secondary emission factor δ for each dynode. The charge collection
efficiency for the ith dynode located within the dynode chain is defined as

no. electrons collected by dynode i


ηi = , (14.54)
no. electrons emitted from dynode i − 1

and the secondary emission factor for the same dynode is defined as

no. electrons emitted by dynode i


δi = . (14.55)
no. electrons collected by dynode i

Suppose that η1 is the charge collection efficiency of the first dynode for those electrons initially ejected
from the photocathode Npc , then the average number of electrons emitted by the first dynode N1 is

N1 = Npc η1 δ1 . (14.56)

For a PMT with M number of dynodes, each with its own charge collection efficiency and secondary emission
factor, the total number of electrons collected at the anode is

Na = Npc (η1 δ1 )(η2 δ2 ) . . . (ηM−1 δM−1 )(ηM δM )ηa , (14.57)


600 Light Collection Devices Chap. 14

where ηa is the final charge collection efficiency of the anode. From Eq. (14.53), the average total gain is

Na )M
G= = ηa (ηi δi ). (14.58)
Npc i=1

The emission coefficient is strongly dependent upon the accelerating voltage, for it is the accelerating
voltage that determines the energy of the electrons that strike the dynode. Further, the electron trajectories
are also strongly dependent upon the applied voltage. In both cases, the overall dynode gain, ηi δi , increases
with interdynode voltage, and can be generally described by

Gi = ηi δi = ki Viα , (14.59)

where ki is a proportionality constant and Vi is the voltage applied between dynode i − 1 and i. Insertion of
Eq. (14.59) into Eq. (14.58) gives the PMT gain as

Qa )M
G= = ηa (ki Viα ). (14.60)
Qpc i=1

Values of α are typically reported between 0.6 and 0.8. Equation (14.60) is often simplified with the
assumption that ηi and ηa are unity, i.e., 100% collection efficiency, and that δi and the interdynode voltages
Vi are identical for all dynodes. With these assumptions Eq. (14.60) reduces to

Na
G= = δ M = (kVdα )M . (14.61)
Npc

where Vd is the voltage applied to each dynode. Note that the assumptions used to derive Eq. (14.61) are
not applicable to all PMTs. For instance, the interdynode voltage is often divided such that the highest
possible η and optimum δ are achieved and this voltage is not always identical for each interdynode spacing.

Example 14.3: Given a 10-stage PMT where all ηi = 0.97, ηa = 0.98, δi = 3.5 for the first 5 stages, and
δi = 4.2 for the last 5 stages, determine average gain for a single photoelectron.

Solution:
The gain is calculated from Eq. (14.60) as
 5   10 
)M
10
) )
G = ηa (ηi δi ) = (ηa )(ηi ) δi δi = (0.98)(0.97)10 (3.5)5 (4.2)5 = 4.96 × 105 .
i=1 i=1 i=6

14.1.7 Factors Affecting the Performance of a PMT


The performance of a PMT is affected by properties such as tube size, the glass enclosure, response speed,
transit time spread (TTS), dark current, optimum wavelength, operating voltage, number of stages, and
gain. These properties are usually reported by commercial manufacturers. However, there are other factors
that affect the performance of PMTs such as dynode glow, space charge accumulation, and environmental
effects. Summarized in the following subsections are descriptions of these other properties.
Sec. 14.1. Photomultiplier Tubes 601

Commercial Specifications
Depending on the intended PMT usage, an operator must select the PMT that works best with the scintillator
of choice. For instance, the sensitivity of the PMT must match well to the emission spectrum of the scintillator
and the timing of the response speed must also match the decay constant of the scintillator. If the PMT has
significant wavelength mismatch, then the overall gain and energy resolution suffer, whereas space charge
build-up and spectral crowding occur for slow PMTs matched to high-speed scintillators. The reader is
directed to Table 14.8 for a list of specifications for some PMTs used in radiation detection.

Dark Current and Noise


The dark current of a PMT is the current that flows in the cathode or anode circuits in the absence of light.
The dark current flow of electrons is a source of random electromagnetic fields that add to electronic noise.
The current that flows to the anode in total darkness has three main origins, namely (a) leakage current on
the PMT surfaces, (b) intermittent emission of electrons, and (c) regenerative effects. The causes of these
dark current contributions vary greatly with the operating conditions and also the prior storage conditions
of the PMT. The dark current is dominated by leakage current under low voltage conditions, by thermionic
emission at typical operating voltages, and by regenerative effects at higher voltages. These components are
discussed in more detail below.

Ohmic Leakage Leakage current, sometimes referred to as “ohmic leakage,” refers to current flow across
the glass envelope and insulators when the PMT has voltage applied to it. Under dark conditions, it
can be recognized by its nearly linear increase as the applied voltage is increased linearly. Although the
leakage current is usually small, there may be residual conductive material remaining in the PMT from the
photocathode and dynode manufacturing process. This residual material becomes an intrinsic property of
the device. A controllable source of leakage current is surface contamination, which may be a result of water
vapor, dirt, grease, or other foreign material that provides conduction paths. Thorough cleansing of the
PMT with isopropyl alcohol (2-propanol) can eliminate such contaminants and reduces this portion of the
leakage current. In humid environments, high voltage may cause arcing between electrodes. Precautions
may be taken to insulate the base connectors with moisture resistant coatings. Most commercial scintillation
detectors come as a single hermetic sealed unit, as a detector and PMT (see Fig. 14.3), thereby eliminating
the arcing problem. Overall, the ohmic leakage current dominates the dark current at low voltages and also
at low temperatures.

Thermionic Emission A thermally dependent source of sporadic electrons is thermionic emission of elec-
trons from the surfaces of the photocathode and dynodes. The current density from thermionic emission,
without gain, is described by Eq. (14.18). From Eq. (14.18), it is found that lowering the work function
of photocathode materials increases thermionic emission. Hence, photocathode materials designed for low
energy (extended red) photon sensitivity have a higher thermionic emission current. At low voltage, the
thermionic emission current is negligible; however, once the voltage is sufficiently high to amplify the cur-
rent through secondary electron emission, the thermionic current contribution becomes important. As the
voltage is increased, thermionic emissions eventually dominate the dark current. Electrons emitted from the
photocathode experience the entire gain described by Eq. (14.61), whereas electrons emitted from any one of
the dynodes have the gain reduced by the number of dynodes skipped in the chain. Also, the photocathode
surface is usually much larger than the dynode surfaces. As a result, most of the overall thermionic dark cur-
rent comes from the photocathode emissions. Because the overall current increase is a function of the PMT
gain, the thermionic current appears to also increase in proportion to the PMT gain. Thermionic emission
from common photocathodes may range between 10−19 to 10−15 amps cm−2 over the maximum sensitivity
range between 300 and 500 nm. For extended red photocathodes, such as the AgOCs S-1 response (see
Table 14.2 and Fig. 14.15), thermionic emission can exceed 10−13 amp cm−2 . Finally, because thermionic
602 Light Collection Devices Chap. 14

Table 14.8. Typical properties of some semitransparent PMTs recommended for scintillation
detector spectroscopy. Data are from ADIT 2016; ET 2016; Hamamatsu 2016.
A B D E F G H I J K L M N O P Q

A L13D21H KCs 13 B 1.49 ∼370 NR 0.8 800 1100 < 1.0 L-10 80 NR NR
A L13B03W KCs 13 S 1.523 ∼385 25 1 NR 1100 < 1.0 L-10 80 NR NR
A B29B01W KCs 28.6 S 1.523 ∼385 25 1 700 1500 0.05 B-11 80 15 NR
A B29B10W KCs 28.6 S 1.523 ∼385 25 1 700 1500 0.05 B-11 80 15 NR
A B38D01W KCs 38.1 S 1.523 ∼385 25 1 NR 1500 10 B-10 80 15 NR
A B51D01W KCs 50.8 S 1.523 ∼385 25 1 1100 1500 10 B-10 80 15 NR
A B51D03W KCs 50.8 S 1.523 ∼385 25 1 1100 1500 10 B-10 97 15 NR
A B76D01W KCs 76.2 S 1.523 ∼385 25 1 1100 1500 10 B-10 97 ∼20 NR
A B89D01W KCs 88.9 S 1.523 ∼385 25 1 1100 1500 10 B-10 97 ∼20 NR
A B133D01W KCs 133.4 S 1.523 ∼385 25 1 1100 1500 10 B-10 97 ∼20 NR
E 9106B RbCs 29 B 1.49 380 28 0.01 500 1200 0.02 L-7 NR 4.5 26
E 9112B RbCs 25 B 1.49 380 25 0.6 1000 1800 0.02 C-10 NR 1.8 20
E 9266B KCs 51 B 1.49 380 30 0.6 850 1100 0.3 L-10 NR 4 40
E 9269B RbCs 51 B 1.49 380 26 0.5 1100 1400 1.0 L-9 NR 7.5 42
E 9490B RbCs 130 B 1.49 380 26 0.6 1100 1600 2.0 L-10 NR 13 60
E 9807B KCs 51 B 1.49 370 30 7.0 1650 2300 3.0 L-12 NR 2 41
E 9813B KCs 51 B 1.49 370 30 70.0 2100 2500 10.0 L-14 NR 2 46
E 9845KB KCs 38 B 1.49 380 28 0.8 1000 1800 0.1 C-10 NR 5 35
E 9900B RbCs 29 B 1.49 370 26 2.5 800 1100 0.3 B-11 NR 15 85
E 9903KB RbCs 38 B 1.49 380 28 0.2 1000 1100 0.1 L-10 NR 3.5 30
E 9924B RbCs 29 B 1.49 380 26 2 900 2000 0.2 B-11 NR 15 85
H R329-02 B 51 B NR 420 NR 1.1 1500 2700 6 L-12 85 2.6 48
H R647 B 13 B NR 420 NR 1.0 1000 1250 1.0 L-10 80 2.1 22
H R877 B 127 B NR 420 NR 0.42 1250 1500 10.0 B-10 88 20 115
H R877-01 B 127 K NR 420 NR 0.42 1250 1500 10.0 B-10 88 20 115
H R878 B 51 B NR 420 NR 1.0 1250 1500 5.0 B-10 90 7 70
H R1306 B 51 B NR 420 NR 0.27 1000 1500 2.0 B-8 95 7 60
H R1307 B 76 B NR 420 NR 0.27 1000 1500 2.0 B-8 95 8 64
H R1450 B 19 B NR 420 NR 1.7 1500 1800 3.0 L-10 88 3 19
H R1635 B 10 B NR 420 NR 1.0 1250 1500 1.0 L-8 80 0.8 9
H R1924A B 25 B NR 420 NR 2.0 1000 1250 3 C/L-10 85 1.5 17
H R2059 B 51 Q NR 420 NR 20 2500 3000 50 L-12 85 1.3 28
H R6091 B 76 B NR 420 NR 5.0 1500 2500 10 L-12 85 2.6 48
H R6234 B H 55 B NR 420 NR 0.27 1000 1500 2 B/L-8 95 1.3 52

A: Manufacturer∗ (A: ADIT, E: ET Enterprises, H: Hamamatsu).


Burle and Photonis no longer make PMTs. ADIT manufactures portions of their former line.
B: Model
D: Photocathode material (B: bialkali, M: multialkai, otherwise by response or chemical name)
E: Window size in mm (H: hexagonal, otherwise round)
F: Window glass (B: borosilicate, K: low 40 K borosilicate, Q; quartz, S: Schott B270)
G: Index of refraction
H: Wavelength of maximum response (nm)
I: Quantum efficiency at optimum wavelength (%)
J: Gain at recommended operating voltage (in units of 10−6 , i.e., J×106 )
K: Recommended operating voltage (V)
L: Maximum operating voltage (V)
M: Typical anode dark current (nA)
N: Dynode type and number of stages (B: box & grid, C: circular cage, L: linear)
O: Cathode radiant sensitivity at optimum wavelength (mA/W)
P: Anode rise time (ns)
Q: Transit time (ns)
NR = not reported
Sec. 14.1. Photomultiplier Tubes 603

emission is also a function of temperature, the thermionic effect can be reduced by cooling the PMT during
operation.
Background Radiation Another contribution to dark current is due to background radiation from external
and internal sources. When cosmic rays, primarily protons and alpha particles, interact with the Earth’s
atmosphere, they can produce a shower of secondary ionizing particles, composed mainly of neutrons, pions,
positrons, and muons. Intersection of these particles with the PMT glass envelope can produce C̆erenkov
radiation, which can subsequently cause photoelectron emission from either the photocathode or the dynodes.
Because significant energy is released from by C̆erenkov radiation interactions, a pulse from such an event
can be significant. C̆erenkov radiation is emitted in a conical shape along the direction of the particle
trajectory; hence dark current from C̆erenkov radiation events is higher for a PMT pointing upwards rather
than downwards.
Radioactive contaminants in the PMT glass envelope (mainly 40 K) can also cause electron emission from
the photocathode and dynodes. Some commercial vendors offer PMTs with low concentrations of potassium
in the glass envelope by using fused silica, for example, to reduce the intrinsic radiation background. Finally,
radiation emitted by building walls and floors, again usually from 40 K and perhaps from other radioactive
sources in the vicinity, can add to spurious counts and dark current. Usually direct interaction of background
radiations with the PMT structure are rare and, thereby of little consequence. Background suppression
becomes important for situations requiring low background counting, and perhaps for liquid scintillation
counting in which the scintillation light output can be relatively small.
Exposure to Ambient Light Exposure of a PMT to normal lighting conditions while under operation can
cause catastrophic damage to the PMT and, consequently, should always be avoided. However, exposure to
typical lighting conditions, even while the PMT is not under bias, can cause an extended, but temporary,
increase in anode dark current. This increase is a consequence of exciting the photocathode, glass envelope,
and internal parts of the PMT, which may phosphoresce over an extended period of time. The intensity and
length of the exposure dark current is a function of the exposure wavelength and exposure duration. Dark
current produced by ambient light exposure decays somewhat exponentially with time. Exposure to short
wavelength photons can cause exposure dark currents over two orders of magnitude higher than exposure to
longer wavelength photons. Even a short burst from an intense source of UV photons can cause appreciable
temporary dark current. PMTs stored in sunlight may need several days in complete darkness before the
dark current is reduced to the usual unexposed condition. Overall, unused PMTs should always be stored
in total darkness and never subjected to intense light, even while not in use.
Regenerative Effects Regenerative effects normally appear at potentials exceeding the recommended op-
erating voltage of the PMT. These include field emission, afterpulsing, dynode glow, glass charging, and
helium penetration. Operation with voltages in which regenerative effects appear can permanently damage
a PMT.
Field emission occurs at irregularities and pinnacles formed on the photocathode and dynode surfaces.
A strong electric field is formed at these points, thereby promoting the emission of electrons. The theory for
this emission was first addressed by Fowler and Nordheim [1928]. Later this theory was modified to include
the Schottky barrier effect and introduced two approximations to the Fowler-Nordheim model to make the
emission model more numerically tractable [Spindt et al. 1976]. In this revised model, the current density J
(A/cm2 ) of emitted electrons is given by
AE 2 φ3/2
J exp −B v(y) , (14.62)
φ E
where A = 1.4 × 10−6 and B = 6.87 × 107 are constants, φ is the work function in eV, E is the electric field in
V/cm, and y is the Schottky lowering of the work function barrier. Finally, the function v(y) is approximated
604 Light Collection Devices Chap. 14

by v(y)  0.95 − y 2 . Note that the applied electric field has a substantial effect on field emission, with a
combined exponential and E 2 increase. Field emitted electrons can fluoresce the surfaces inside the PMT,
causing emissions of photons that may reach the photocathode. Field emission can also cause permanent
damage and significantly shorten the life of a PMT.
Afterpulsing is the production of minor spurious pulses following a main event. There are two main
sources of afterpulsing, luminous and ionic [Morton et al. 1967; Krall 1967]. Luminous afterpulses are
produced by energetic electrons causing the anode or dynodes to fluoresce. Fluoresence photons can travel
back to the photocathode and cause a subsequent event, usually lower in magnitude than the main event.
Luminous afterpulses are delayed by the sum of the electron and fluorescent light transit times through the
PMT, typically between 20 and 100 ns.
Ionic afterpulsing is caused by contamination gases in the tube becoming ionized and subsequently striking
the photocathode. The sources of the contamination gases may be outgasing of components, desorption
from the PMT walls, and residual gases remaining after the evacuation process. Energetic electrons drifting
through the PMT can cause ionization of these trace gases, thereby producing positive ions. These positive
ions, having much lower mobility than electrons, drift much more slowly than do electrons and, hence, strike
the photocathode with a delay between 200 ns to over 1 μs. When these ions strike the photocathode, they
can release numerous secondary electrons, which in turn produce another electronic avalanche and pulse.
The magnitude of an ionic afterpulse is a function of the positive ion kinetic energy; hence the ionic afterpulse
magnitude is strongly dependent upon the applied voltage. Troubling gas ions include N+ +
2 and H2 , and gas
sources may include N2 from residual air and detachment of H2 from water moisture. Under some conditions,
CH+ +
4 and He may be present, also causing afterpulsing. Modern manufacturing procedures are set in place
to reduce the concentration of these residual gases. For ordinary scintillation counting and spectroscopy,
afterpulsing is usually of little consequence. However, for measurements requiring critical timing information,
afterpulses can prove to be an annoyance. Techniques to suppress afterpulses are described in the literature
[Lamaze et al. 1975; Mirzoyan et al. 1997].
If the PMT is operated or stored in an environment with high He concentrations, it is possible for the
He to diffuse through the glass or connecting regions into the PMT enclosure. Because He is a non-reactive
inert gas, He does not attach to the PMT structure, hence is not gettered. As He concentrations build, it
may become a problem by producing afterpulsing when ionized. Relatively high concentrations of He+ can
cause electrical breakdown, and ultimately, render the PMT useless.
At high enough operating voltages, electron bombardment upon the dynodes can cause the emission of
light, recognized as a blue glow, and occurs particularly in the latter stages of the dynode chain. Photons
from this dynode glow can scatter back to the photocathode, thereby becoming an additional source for
noisy current [Krall 1967]. This effect is largely suppressed by including shields in the PMT that work to
block light from reaching the photocathode.
Acceleration of electrons, or ions, into the PMT glass envelope can produce the photoemission of sec-
ondary electrons, an effect referred to as glass charging. This particular problem occurs if the glass envelope
has a positive potential that competes with that of the anode and can arise from external voltage sources.
Installation of shielding material around the PMT reduces the problem of glass charging. The conductive
shield should be grounded to the same potential as the cathode; otherwise, should the shield maintain a
positive potential, there is a risk of permanently damaging the PMT [Engstrom 1980].

Timing
The timing characteristics reported for PMTs are the transit time, rise time, fall time (or decay time), and
statistical spread. The transit time is the time between a delta-function light pulse striking the photocathode
and when the output current from the PMT reaches peak amplitude [Frank 1977], as shown in Fig. 14.29.
Sec. 14.1. Photomultiplier Tubes 605

The transit time has many components,


including the diffusion time required for elec- Transit Time
trons excited in the photocathode material Rise Fall
to reach the vacuum interface, the time for Time Time
electrons to transverse the space between
the photocathode to the first dynode, and Input Excitation
Output
the multiple transverse times between dyn- Pulse
90%
odes. Emission times for common alkali
metal emissive materials is about 10 ps.
FWHM
However, the diffusion times of NEA materi-
als, because of the longer electron mean free 50%
paths, may extend beyond 100 ps. Yet, these
emission times have little consequence com- 10% Time
pared to collection times between dynodes.
The longest transit time component is usu- Figure 14.29. The different time constants used to characterize the
ally the time required for electrons to travel output pulse from a PMT produced by a delta-function input.
from the photocathode to the first dynode.
This is especially true for configurations with large photocathode surfaces because large photocathodes must
be placed further away from the dynodes to allow efficient focusing of electrons.
The rise time of the PMT is mean time required for the output pulse to increase from 10% maximum to
90% maximum. It is the charge density and the charge collection time measured between the last dynode
and the anode that determines the rise time, mainly because the anode output current is induced almost
entirely from charges drifting between these last two electrodes (see Sec. 8.5 on weighting potentials). Rise
times for common PMTs range between 1 and 20 ns. The PMT rise time is typically smaller than the fall
time, and provides higher accuracy for timing measurements. The fall time of the PMT is the mean time
required for the trailing edge of the output pulse to fall from 90% maximum to 10% maximum.
The statistical time spread is the full width at half maximum (FWHM) of the PMT output pulse.
Contributions to statistical spread time include the time spread of the scintillation light source, time spread
in electron trajectories from the photocathode to the first dynode, and time spread in the multiplication
process as electrons move through the dynode chain. The light source time spread is a function of the decay
time for the scintillation process, a physical process that cannot be altered for a given scintillation material.
The time spread for electrons traveling between the photocathode and the first dynode can be minimized
by including a curved inner photocathode, thereby providing nearly equidistant electron trajectories. The
time spread from secondary electron emission between dynodes is complicated by the differences in electron
emission speeds and directional trajectories. Overall, the timing resolution is determined mainly by the
statistical spread in the secondary electron emissions.
The speed of an electron reaching a dynode is directly proportional to the applied electric field or voltage
between the adjacent dynodes. Hence, the transit time is inversely proportional to voltage. Consequently,
the time spread of electrons between dynodes is dependent on 1/Vi where Vi is the voltage between dynodes
i − 1 and i. If it is assumed that the speeds of electrons
√ reaching a dynode have a Gaussian distribution, the
standard deviation in speeds is proportional to 1/ Vi . Hence, the broadening of the output pulse decreases
with increasing voltage, and the timing characteristics of a PMT are usually maximized at the highest
recommended operating voltage.
Fluctuations in the transit time between pulses, referred to as jitter, determines the accuracy limit for
timing measurements. The variance in the transit time for a delta-function light input is described by

2
σtt = σ12 + σ22 , (14.63)
606 Light Collection Devices Chap. 14

where σ12 is the variance for the cathode-to-first-dynode collection time, and σ22 is the time variance of the
combined collection times for the remaining interdynode spacings. The variance σ12 has several contributions,
mainly, absorption depth variance, emission location/trajectory variance, and chromatic variance. The vari-
ance in absorption depth affects the variance in the energies of the emitted electrons. Electrons that must
diffuse far to the vacuum interface may have barely enough energy to surmount the energy barrier, whereas
electrons excited at the vacuum interface may be emitted with the total residual energy φ − hν. These elec-
trons are emitted into the vacuum envelope in various directions, some directly towards the first dynode and
others at varying angles away from the first dynode. Additionally, the emergence point on the photocathode
may be anywhere on its surface. All together, the different diffusion times for the photoelectrons to reach the
surface of the cathode and the different emergent locations and directions determine the variance in the time
required for an electron leaving the photocathode surface to reach the first dynode. Wavelength variance is
of little consequence for monochromatic light; however, scintillators emit light over a spectrum of energies,
thereby adding to the variance in photoelectron energies.
Suppose a single electron is released from the photocathode. If the interdynode characteristics are
assumed identical, then the variance in collection time between the dynodes as a function of transport
between dynodes is [Gatti and Svelto 1966],
2
σt1 σ2 σ2 σ2
σd2 = + t22
+ t33
+ . . . + tM , (14.64)
δ δ δ δM
2
where σti is the variance in flight times from dynode i − 1 to dynode i and the last term is the contribution
to the flight time from the last dynode to the anode. Note that the last term is generally negligible, mainly
because of the large value of δ M and that charge induction only initiates as electrons travel towards the
anode from the last dynode. If, in addition to the assumption that δi = δ for all dynodes, one also assumes
σti = σt for all dynodes, then for large values of M , Eq. (14.64) reduces to,

σt2
σd2  . (14.65)
δ−1
If the variance in gain is also included, then Gatti and Svelto [1966] show that the collection time variance
for the dynode bank is,  
σt2 1 σt2 δ
σ2 
2
1+ = . (14.66)
δ−1 δ−1 (δ − 1)2
The total variance in the transit time, given by Eq. (14.63), is

2 σt2 δ
σtt = σ12 + . (14.67)
(δ − 1)2

Substitution of Eq. (14.59) into Eq. (14.67) yields,

2 σt2 kV α
σtt = σ12 + , (14.68)
(kV α − 1)2

which for large voltages reduces to


σt2
2
σtt  σ12 + . (14.69)
kV α
This result clearly shows that an increase in the operating voltage decreases the fluctuations in the transit
time.
Sec. 14.1. Photomultiplier Tubes 607

For typical scintillation spectroscopy with relatively slow inorganic scintillators, such as NaI:Tl, most
PMTs have sufficiently fast responses that the time response of the photomultiplier is inconsequential com-
pared to the decay time of the scintillator. However, with recent advances in producing scintillators with
fast decay times, the transit and rise times of the PMT become important. Hence careful selection of a
fast PMT is important for these short decay-time scintillators. In the case that a slow PMT is used with a
relatively fast inorganic scintillator, such as LaBr3 , the high density of charge in the PMT can cause serious
gain distortions and non-linear behavior, thereby distorting the resulting pulse height spectrum.
Photocathode Non-uniformities
The photocathode coating usually has non-uniformities across the surface that produce a variation in light
response across the photocathode. For radiation spectroscopy, scintillation light striking different regions
of the photocathode can produce a varied response, thereby degrading energy resolution. For PMTs with
large photocathode surfaces, usually used for radiation detection applications, the light response decreases
abruptly near the photocathode periphery. Scanning measurements across the surface of PMTs indicate that
the variance is relatively small for well-processed photocathodes (± 3%) [Engstrom 1980]. This variation in
response is usually least at the optimum peak wavelength, but can be much larger and erratic as the photon
wavelength is increased from the optimum wavelength.
There are still two principal reasons for the non-uniform photon response: (1) variations in the photo-
cathode layer thickness produced by the physical vapor deposition used to form the coating, and (2) the
design of the electron optics used to guide the photoelectrons to the first dynode. Light response uniformity
is improved by producing a diffusive layer at the glass/photocathode interface, accomplished by sandblasting
the inner surface of the glass before the photocathode material is applied. Light is scattered over a wider
area, thereby decoupling the point of intersection from the overall photoresponse. Other methods to decrease
the effects of photocathode non-uniformity include the installation of a permanent ring magnet or solenoid
around the photocathode, thereby defocusing electron emissions around the periphery and nullifying their
contributions. Also, placing a stopped-down aperture between the scintillator and photocathode reduces
the sensitive photocathode region that contributes to the photocurrent and, thereby reduces effects from
photocathode non-uniformities.

14.1.8 Ancillary Equipment


Support equipment needed to operate a PMT properly include the tube base, output electronics, and shield-
ing. This ancillary equipment is briefly discussed in this section. Photomultiplier specification sheets typically
provide a recommended socket and voltage divider configuration that is dependent on the PMT application.
The socket serves as an electrical connector to the PMT dynode pins. Although separate sources can be used
to provide voltage to each PMT dynode stage, such a configuration is somewhat impracticable. Instead, the
applied high voltage is usually divided amongst the focusing electrodes, the anode, and the dynodes.
Sockets and Voltage Dividers
PMTs have various electrical pin configurations; hence, matching the PMT to the proper socket is, of course,
mandatory. These sockets can be acquired with or without mounting flanges, depending on the intended
application. For instance, the mounting flange allows the PMT to be installed on a stand-alone base, whereas
sockets without the mounting flange must be connected directly to a circuit board. The preferred voltage
divider can be connected directly to the socket and changed according to application.
Voltage Divider There are two basic types of voltage dividers, namely, resistive and active types. The
resistive dividers consist of a series of resistors that divide the voltage between the electrical parts of the
PMT. Of these, there are three main types of resistive divider: the uniform type, the progressive (or tapered)
type, and the intermediate type. After the initial region between the photocathode and the first dynode,
608 Light Collection Devices Chap. 14

cathode anode
focus ..........
d1 d2 d3 dM-3 dM-2 dM-1 dM

C
A
RL
+V
ri ri ri ri ri ri ri ri ri ri ri ri ri ri

cM-4 cM-3 cM-2 cM-1 cM

cathode anode
focus ..........
d1 d2 d3 dM-3 dM-2 dM-1 dM

A
RL
ri ri ri ri ri ri ri ri ri ri ri ri ri ri
-V cM-4 cM-3 cM-2 cM-1 cM

Figure 14.30. Voltage divider configurations with (top) positive high voltage applied to the
anode, grounded cathode, and with series decoupling capacitors, and (bottom) negative high
voltage applied to the cathode, grounded anode, and with parallel decoupling capacitors.

the uniform divider distributes the applied voltage equally over the dynodes stages. The uniform divider
yields the highest gain of the three types of dividers, and is the most frequently used configuration for
radiation measurements. The progressive divider increases the applied dynode voltage in the direction of the
anode. The progressive divider helps overcome space charge effects and non-linear behavior for high current;
however, the gain is typically lower than that of uniform dividers. Finally, the intermediate divider applies
the same voltage to the first several dynodes stages, but then provides progressively larger voltages to the
latter dynode stages. Intermediate dividers are used for fast response PMTs.
An active divider consists of a string of high impedance resistors connected in parallel with a string of field
effect transistors [Kerns 1977; ET 2011]. These transistors help regulate the voltage between the dynodes
to keep the potential drop constant. An active voltage divider ensures constant gain up to the maximum
allowable current (about 100 μA). Power consumption is low, about 100 mW, so that portable PMTs can
be realized. Active dividers often have current limiting circuitry to prevent damage to the PMT. An ideal
active divider can sense the dynode voltages over the entire PMT dynamic range.
The applied PMT high voltage is often a positive bias applied to the anode with the photocathode region
grounded. However, the PMT can work equally well with negative high voltage applied to the cathode with
the anode grounded, as shown in Fig. 14.30. Specifications made by PMT manufacturers give the preferred
bias arrangement along with recommended voltage dividers and sockets. The applied high voltage is often
positive, thereby allowing the glass envelope and photocathode to remain at zero potential. One benefit of
applying positive high voltage is the suppression of spurious pulses from glass electroluminescence. Further,
Sec. 14.1. Photomultiplier Tubes 609

it is typical that a scintillation crystal attached to the PMT be at zero potential, and the positive high voltage
configuration practically eliminates spurious pulses from high-voltage leakage to nearby grounded objects.
However, there are important cases when negative high voltage is preferred. With negative high voltage,
the coupling capacitor at the output is no longer necessary because the anode is grounded. This divider
then allows the resistive divider and PMT to be directly coupled to the output circuitry. The negative bias
configuration is used for fast pulse applications in which the output is impedance matched to the transmission
line, and for current mode operation with DC-coupling.
Decoupling Design of the resistive divider circuit depends upon the high voltage supply, the required
voltage distribution, and the expected anode current (characterized by the FWHM of the output pulse).
Variations in anode output current can be minimized by ensuring that ileak /iA ≥ 100, where iA is the anode
output current and ileak is the leakage current flowing through the resistive divider [Flyckt and Marmonier
2002]. The leakage current associated with the diode divider circuit can be estimated as
&
N
ileak  Vbias ri (14.70)
i=1

where the ri are the resistances of the divider.

Example 14.4: Consider a 10-dynode PMT with a normal operating gain of 105 at 1000 volts potential
and an anode output current FWHM of 10 ns. For a uniform resistive divider in which the voltage drop
between the photocathode and the first dynode is five times the interdynode potentials, what is the minimum
resistance required for each resistor in the divider?

Solution:
A single electron escaping the photocathode produces 105 photoelectrons. The anode current produced
by a single electron is then,

qG (105 )(1.6 × 10−19 C/e− )


iA = = = 1.6 μA.
tA 10−8 s

where G is the gain and tA is the anode rise time. Conforming to the recommendation that ileak /iA ≥ 100,

ileak ≥ 100 iA ≈ 160 μA,

and the total resistance must be


 (1000 V)
ri = = 6.25 MΩ.
i
(160 × 10−6 A)

With 9 dynodes and the photocathode space, the voltage divisor is 9 + 5 = 14, so that the interdynode
resistance must be at least 446.43 kΩ.

Although high resistances can be employed, it is far more usual to use capacitors to decouple the dynodes
from the resistive divider circuit. By so doing, the instantaneous anode current, or the currents between the
dynode stages, can greatly exceed the average divider current. Decoupling may be accomplished by inserting
capacitors either in parallel or series with the divider circuit resistors. Either configuration works; however,
capacitors arranged in parallel require much higher voltage ratings. These decoupling capacitors function as
610 Light Collection Devices Chap. 14

charge storage to make up for the current drain from the voltage source as the electron cascade progresses
through the PMT.
Suppose that the maximum allowable change in voltage at any dynode is ΔV and the expected anode
current is
iA = nqe GtA , (14.71)
where n is the number of photoelectrons. Then the decoupling capacitance for the last dynode is
nqe G
CM = . (14.72)
ΔV
where M is the number of dynodes. Consider the case in which all dynode gains are equal; then the required
limiting capacitance for each dynode stage is,
nqe G CM
Ci = = M−i , (14.73)
δi ΔV δi
where Ci and δi are the decoupling capacitance and gain from dynode number di , respectively. Typically, a
safety margin equivalent to the stage gain is multiplied by the capacitance to yield,
CM CM
Ci = δ N −i
= N −i−1 . (14.74)
δi δi
for all coupling capacitors except CM . In most cases these decoupling capacitors are needed only if the
required Ci is greater than the dynode stage capacitance (about 20 pF). The first several stages do not need
decoupling capacitors, consequently only the latter stages of the divider circuit require these decoupling
capacitors.
Preamplifier
Commercial scintillation/PMT units often come with a preamplifier, not to be confused with the voltage
divider. In some circumstances, the output pulse may be large enough without further amplification, or the
application may require current mode operation rather than pulse mode operation. However, for typical
radiation detection measurements, it is important to amplify and shape the output pulse from the PMT.
The preamplifier provides a small amount of gain, shape the output pulse (typically a tail pulse), and couple
the PMT to the main amplification electronics for pulse mode operation.
Magnetic Shield
Photomultiplier tubes are affected by external magnetic and electrostatic fields because such fields can
deflect the electrons from their designed trajectories. The end result is a loss of gain, and for radiation
spectroscopy, deterioration in energy resolution from increased statistical spread of photoelectrons reaching
the first dynode. Magnetic field effects generally become smaller as the high voltage increases, but usually
not enough to eliminate the performance degradation of the PMT. In short, PMTs must be shielded against
magnetic fields. Obviously, because the electrons within the tube are guided through successive potentials,
external electric fields must also be shielded from the PMT. Most often the PMT is wrapped with “mu-
metal” to terminate these fields and prevent them from interfering with the electron trajectories.11 To
prevent problems with glass charging and electroluminescence, the magnetic shield is kept at the same
potential as the photocathode. Note that operation with the magnetic sleeve shield held at a high voltage
(the situation when the cathode is operated at high voltage) presents a special safety issue, and precaution
should be exercised to prevent hazardous shock. Preformed sleeves of mu-metal are usually available from
the PMT manufacturers.
11 The name “mu-metal” comes from the Greek letter μ, the usual symbol for magnetic permeability.
Sec. 14.2. Semiconductor Photodetectors 611

14.1.9 Environmental Effects


Finally, a word or two regarding environmental effects on PMTs. Most manufacturers specify maximum
storage and operating temperatures, which according to Engstrom [1980] is usually near 75◦ C. Apparently,
higher temperatures can cause a chemical reaction at the photocathode which may compromise the PMT
performance. On the other hand, rapid cooling may fracture the glass envelope. Differences in the thermal
expansion coefficient between the glass and PMT socket/base may also cause cracking, and it is recommended
that the PMT temperature not go below −50◦ C. Cooling may also produce condensation that may cause
short circuits between the dynodes. Coating with a moisture-resistant insulator can help mitigate this
problem.
Photomultiplier tubes can withstand reasonable pressures, but it is advised that the external pressure be
kept below 3 atm to avoid possible implosion.12 Recall that gas diffusion into the PMT from a high pressure
environment may be a problem, especially with He gas. Also photomultiplier tubes generate heat; hence
operating them in vacuum can be problematic if a heat sink is not employed.
Photomultiplier tubes are relatively fragile, but can survive some level of shock force (up to about 10
g). Special robust PMTs are designed to withstand high shock (some up to 1500 g), and are used for space
applications, military applications, and oil well logging. However, careful handling is always recommended.
Damage to the internal structure can cause shorting or loss of gain and other performance characteristics.
Obviously, excessive shock may also crack the glass envelope.
Of course, photomultiplier tubes are widely used in a radiation environment. High radiation environ-
ments, however, can cause an increase in background current by the production of fluorescence in the glass
envelope, particularly in the face plate adjacent to the photocathode [Johnson 1973]. Permanent damage oc-
curs from high radiation exposures that cause browning of the PMT faceplate. Soda lime and LiF faceplates
are very susceptible to such radiation damage. Borosilicate glass has only slightly more radiation hardness.
Quartz and sapphire windows show much less degradation than borosilicate or soda lime glasses. For shorter
wavelength UV photons beyond the range of quartz or sapphire, MgF2 windows are recommended for use in
high radiation environments.

14.2 Semiconductor Photodetectors


Semiconductor photodetectors are based upon physics discussed in Chapters 12, 15, and 16, which include
solid state physics, semiconductor device physics, and semiconductor device configurations. However, for
completeness, the authors decided that these important photosensitive devices should be covered, to some
extent, in the present chapter. Hence, a general explanation of these photodetectors and their operation is
provided here, whereas detailed explanations on how these devices are designed and operated are offered in
Chapters 15 and 16.
Attractive features of semiconductor photodetectors include their compact size, relatively low operat-
ing voltage, and fast response times. Semiconductor photodetectors, unlike PMTs, are also insensitive to
magnetic fields, thereby allowing them to be used in environments with high magnetic fields. The overall
quantum efficiency can be remarkably high for specific ranges of photon wavelengths as determined by the
semiconductor’s band-gap energy and the photon absorption efficiency. The main types of photon detectors
used with scintillators are photodiodes, avalanche photodiodes, and semiconductor photomultipliers.

12 Thiseventuality occurred on a devastating scale on Nov. 12, 2001 in the Super-Kamiokande neutrino detector located 1000 m
below ground in an old zinc mine in Japan. The detector was a cylinder (34 m in diameter and 36 m high) filled with ultra-pure
water and lined with 11,146 PMTs. On the fateful day, as the chamber was being refilled, a PMT imploded setting off a chain
reaction that caused 6,600 of the $3,000 PMTs to also implode.
612 Light Collection Devices Chap. 14

(a) (b) (c)


Figure 14.31. Semiconductor photodiodes of different designs, including (a) a common
pn junction photodiode, (b) a pin photodiode and a (c) Schottky contact photodiode.

14.2.1 Photodiodes
Photodiodes are semiconductor devices formed into a pn or pin junction diode. The designation p refers
to p-type impurity dopants that produce positive charge carriers, n refers to n-type impurity dopants that
produce negative charge carriers, and i refers to the intrinsic material that is generally devoid of impurity
dopants. Diodes formed from a simple pn junction offer an inexpensive method for detecting photons, yet
have relatively thin active volumes. The reason for this thin volume, as explained in detail in Chapter 15,
arises from buidup of space charge in the sensitive region that limits the electric field and, thus, narrows
the photon active sensitive region or depletion region. The n and p doped regions are necessary for the
device to function properly, yet this space charge appears as a consequence of the “impurity doping” in the
semiconductor.
A configuration often used to increase the active region of a semiconductor photodiode is the pin junction
diode. In general, the device has a p-type material adjacent to intrinsic material, with n-type material com-
pleting the diode opposite the intrinsic material. A simple pin device cross section is depicted in Fig. 14.31(b).
The active region is increased by including an intrinsic, or low-doped (π or ν), region between the n and p
region, thereby greatly reducing the space charge density and increasing the active region width.
A simple and common photodiode is based upon the Schottky effect (see Sec. 15.3), in which the appli-
cation of an appropriate metal forms a rectifying blocking contact upon the semiconductor. Such a device
functions similarly to a pn or pin junction photodiode, but generally has higher leakage current. The higher
leakage current is fundamentally due to the physical process that suppresses the leakage current in reverse
bias. The Schottky diode relies upon a barrier to reduce thermionic emission, whereas the pn junction relies
upon the reduction in minority carriers available for leakage as explained in more detail in the next chapter.
When photons strike the semiconductor photodiode, usually fabricated from Si or GaAs based materials,
electrons are excited into the conduction band of the material. A voltage bias across the diode causes the
photoelectrons to drift across the device and induce charge in a similar fashion as that described for gas-filled
ion chambers. The quantum efficiency of the semiconductor diode varies with the configuration and packaging
of the diode. For instance, different commercial Si photodiodes have peak efficiencies at wavelengths ranging
between 700 to 1000 nm. Regardless, they are typically more sensitive to longer wavelengths than commercial
PMTs. For instance, CsI(Tl) scintillation emissions are better matched to Si photodiodes than to PMTs.
Photodiodes operate with low voltage, are small, rugged and relatively inexpensive and, thus, they offer a
compact method of sensing light emissions from scintillators.
Sec. 14.2. Semiconductor Photodetectors 613

Figure 14.32. Optical absorption coefficients for various semiconductor photodetector materials.
After [Melchior 1972; Sze 1981].

Performance Characteristics Quantum efficiency generally approaches a maximum as photon energies


approach the band-gap energy. For photon energies below the band gap energy (hν < Eg ), the material is
generally transparent to the light, except for absorption by defect and impurity centers. For photon energies
greater than the band gap (hν > Eg ), absorption may occur with increasing likelihood as the photon energy
increases. The increase in the absorption coefficient α occurs because electrons that are deeper in the valence
band can be excited across the band gap into the conduction band as the energy of the absorbed photon
increases. This property can be observed in Fig. 14.32 as the increase in absorption coefficient α as the light
wavelength decreases.
For photons with wavelengths below the cutoff wavelength, determined by the semiconductor band-gap
energy, optical absorption increases, as also shown in Fig. 14.32. However, the energy conversion efficiency13
actually decreases as the photon energy increases, a consequence of excess energy being expended to excite a
single electron-hole pair. For example, if an 800 nm photon (1.55 eV) is absorbed in GaAs (Eg = 1.42 eV),
there is a likely chance that a single electron-hole pair is excited; hence ηe = 0.916. The same is true for a
700 nm photon (1.77 eV), but ηe = 0.802. Although the energy is higher for the second case, the photon
has insufficient energy to excite two electron-hole pairs, causing ηe to decrease. Consequently, the energy
conversion efficiency decreases even though the photon absorption efficiency increases.
The active region width of Si pn and pin photodiodes need only be about 1 to 4 microns to effectively
absorb photons of wavelengths ranging between 450 nm to 650 nm [Melchior 1972]. For Ge photodiodes, these
same active region widths correspond to photons of 950 nm to 1500 nm wavelengths. At shorter wavelengths,

13 The energy conversion efficiency ηe is the band-gap energy divided by the energy expended to produce an electron-hole pair,
i.e., ηe = hν/Eg .
614 Light Collection Devices Chap. 14

absorption increases near the surface, consequently causing an increase in surface recombination and, thereby
a decrease in the quantum efficiency. This behavior is apparent in Fig. 14.33 at the shorter wavelengths.
Thus, the long wavelength cutoff is limited by the band-gape energy and the short wavelength cutoff is
limited by high surface absorption and surface recombination. By contrast, Si Schottky contact photodiodes
(also known as metal-semiconductor photodiodes), see Fig. 14.31(c), have thin metal contacts that allow
photons to pass deeper into the active region of the photodiodes than do pn and pin diodes and, thereby
extend the short wavelength range below 400 nm [Melchior 1972].
Both the energy conversion efficiency and the quantum efficiency determine the total charge excited
by scintillation photons and, thereby affect the energy resolution of the detector. Silicon photodiodes can
function at typical scintillation emissions with wavelengths near 400 nm, but excel in performance at longer
wavelengths, generally in the 600 nm to 1000 nm range. Photodiodes generally do not have gain, and the
charge signal is determined by the primary electron-hole pairs excited by the scintillation event. Conse-
quently, the signals from photodiodes are small and need more amplification than signals from PMTs.
The quantum efficiency ηQ is defined as the average number of electron-hole pairs produced per scintil-
lation photon. For light detection, a useful quantity used to determine the relative sensitivity of the diode
to light is the spectral responsivity R, usually measured in amperes/watt [Donati 2000], and is defined as14

qe ηQ λ qe ηQ
R= = . (14.75)
hc hν
From this result, R is seen to decrease with photon energy and to increase with quantum efficiency. Shown in
Fig. 14.33 are spectral responses for several semiconductor photodiodes of interest for scintillation counting.
The details of semiconductor devices and operation are presented in Chapters 15 and 16. However,
briefly stated, the number of charge carrier pairs produced is the average ionization energy w divided into
the particle energy E, i.e., the number of electron-ion pairs is E/w. For high energy photons (x and
gamma rays), most semiconductors have average ionization energies ranging between 2.5 and 5.5 eV/e-h
pair. For low-energy photons emitted from scintillators, the average energy expended per electron-hole
pair is a function of the absorption efficiency, the quantum efficiency, and the energy conversion efficiency.
Consequently, without gain, the total number of charge pairs produced per scintillation event is considerably
less than the number of charges produced by a PMT. Although the statistical spread in the number of
electron-hole pairs produced is less than that predicted by Poisson statistics, the relatively low number of
charge carriers per event compromises the overall energy resolution. Additionally, electronic noise from
leakage and generation current can adversely affect the pulse height spectrum because of the relatively small
signals produced by a common photodiode. This problem of poor energy resolution is particularly severe for
low-energy scintillation photons.
Electronic Noise The electronic noise arising in common photodiodes is classified as either series noise
or parallel noise. It is the fluctuation in these two current sources that produces a broad electromagnetic
spectrum of frequencies in the noise, and, thus, it is usually referred to as white noise.
Parallel noise arises from dark current fluctuations within the diode, generally from thermionic leakage
current and bulk generation current. Bulk generation current arises from charge carriers being thermally
excited from the valence band into the conduction band, a process that increases with the active volume
of the detector. Hence, bulk generation current is a function of both the contact area and the depth of
the active region. Moreover, the dark current increases with applied voltage, mainly because the leakage
current increases from non-ideal current saturation and the generation current increases as the active region
increases with voltage. Parallel noise can be reduced by decreasing the leakage current of minority carriers

14 This property is sometimes referred to as “spectral sensitivity” or “photosensitivity”.


Sec. 14.2. Semiconductor Photodetectors 615

Figure 14.33. Spectral responsivity in amps/watt for various semiconductor photode-


tector materials of interest for scintillation counting. Quantum efficiency is also indi-
cated. [after Donati 2000].

or by increasing the rectifying barrier height. Because the total leakage current increases as the total contact
area increases, the practical size of photodiodes for scintillation spectroscopy is limited. For Si photodiodes,
this area is usually restricted to approximately 1 cm2 .
Series noise arises from fluctuations in the series resistance and fluctuations in the current flowing into
the input stages of the preamplifier circuitry, fluctuations that consequently produce short current bursts in
the output of the preamplifier. This series noise is also referred to as shot noise. A large contribution to the
2
series noise arises from the detector input capacitance Cin and is generally quantified as a function of Cin
[Iwanczyk and Patt 1985]. Hence, it is important to reduce the input capacitance as much as practically
possible. This reduction can be accomplished by both reducing the detector contact area and increasing the
active region, between the contacts. Note that both series and parallel noise can be decreased by selecting
photodiodes with small contact areas; however, parallel noise decreases with the size of the active region
whereas series noise increases with the size of the active region. Such counteracting trends in the two noise
sources means there is an optimum operating voltage, which determines the size of the active region. Indeed,
photodiodes are usually operated at active region depths well beyond those required to completely absorb
the impinging scintillation light in order to optimize performance.
Photodiode Materials Silicon is of interest because of its good quantum efficiency in the extended red-
wavelength range and because it couples well to common scintillators such as CsI(Tl) and even BGO,
scintillators that typically are not optimized when coupled to PMTs. Although most photodiodes are manu-
factured from Si materials, there are many photodiodes manufactured from wide band-gap materials. These
wide bandgap materials are almost all compound semiconductors, such as InP, GaAs, CdTe, GaP, CdS, and
SiC, and generally have lower bulk generation current than that in Si. Further, because of their higher re-
sistivity, wide band-gape semiconductors generally have lower leakage currents than Si diodes. Indeed, dark
616 Light Collection Devices Chap. 14

current can be reduced, in concept, by wider band-gap materials, but this higher resistivity is usually ac-
complished by the purposeful introduction of compensating energy levels into the material. The fluctuations
in generation current can be significant, mainly a result of the shorter generation-recombination lifetimes
characteristic of compensated compound semiconductors, and it is the fluctuation in dark current that con-
tributes to the electronic noise. Wide band-gap experimental photodiodes have also been investigated, such
as HgI2 . Indeed, a rather sizeable CsI(Tl) crystal (about 16 cm3 ) coupled to a HgI2 photodiode held the
energy resolution record for many years for a scintillator/semiconductor device operated at room tempera-
ture, namely 4.98% FWHM at 662 keV [Markakis 1988]. Competing processes between direct gamma-ray
detection by the photodiode and the CsI(Tl) crystal were evident, a consequence of using compound semi-
conductor photodiodes composed of high Z elements. Some other binary compound semiconductors and
complex ternary and quaternary compound semiconductors, such as PbS, PbSe, InSb, InGaAs, InAsSb,
and InGaAsP, have extended IR sensitivity, but typically also have higher dark current densities than those
expected for wide band-gap materials.
Overall, photodiodes offer a relatively compact and inexpensive method to detect radiation induced light
from scintillators. They usually require only a modest bias voltage, compared to that required by PMTs,
and are generally unaffected by magnetic fields. Further, semiconductor photodiodes are robust and less
prone to shock damage. However, semiconductor photodiodes have much smaller output signals, thereby
compromising energy resolution. Parallel and series noise further reduce energy resolution. Finally, the
leakage current from semiconductor photodiodes increases with temperature, thereby reducing their use in
high temperature environments. Compact Peltier coolers can be used to help remedy the noise problem,
yet this added complication with its own power requirement still restricts the use of photodiodes in many
circumstances.

14.2.2 Drift Diodes


One method to increase the active area of a photodiode, while still maintaining relatively low capacitance,
is to use a silicon drift diode (SDD). Details of the structure and operation of the drift diode are given
in Sec. 16.4 on silicon detectors. However, the basic device has a relatively small anode with structured
cathodes guiding electrons by way of consecutively divided potentials. The capacitance is dominated by the
low anode capacitance. Further, modern designs incorporate the first amplifier stage directly onto the diode,
thereby reducing the coupling capacitance. These detectors can have relatively larger areas compared to
common photodiodes, often greater than 25 mm2 and up to 1 cm2 area. Modest cooling (about 0◦ C) can be
implemented to ameliorate the bulk generation current caused by the larger diode volume.
Although the charges drift for a longer time than that in common photodiodes (typically a few microsec-
onds) the rise time is surprisingly fast, mainly because it is mostly dependent upon the drift distance between
the anode and the closest cathode in the structure. However, diffusion of the charge cloud causes differ-
ences in rise times, a consequence of photon interactions occurring randomly over the entire diode volume.
Hence, the diode integration time should be set high enough to allow complete charge collection, regardless
of interaction location.
Drift diodes have demonstrated excellent results when coupled to scintillators. For instance, a cylindrical
CsI(Tl) crystal, (3-mm diameter and 5-mm thickness) produced 4.34% FWHM energy resolution for 662-keV
gamma rays when coupled with Nuclear Enterprises’ 586 optical grease to a SDD [Fiorini et al. 1998]. Later,
Fiorini et al. [2006] produced 2.7% FWHM energy resolution for 662-keV gamma rays with a cylindrical
LaBr3 (Ce) crystal (5-mm diameter and 5-mm thickness) when coupled to a 5 mm2 SDD. Although the
scintillators were comparatively small, the excellent reported performance rivals the best performance for
systems incorporating PMTs. To increase the overall detector area, an array of hexagonal SDDs is also
reported by Fiorini et al. [2007] as a method to produce a compact Anger camera [Anger 1958].
Sec. 14.2. Semiconductor Photodetectors 617

14.2.3 Avalanche Diodes


Semiconductor photodiodes based upon avalanche gain provide a method to combine the high quantum
efficiency of semiconductors with large output signals. Avalanche photodiodes (APDs) are operated at high
reverse bias voltages and are designed such that an electric field capable of promoting avalanche multi-
plication is produced within the device. Those properties, important for common photodiodes used for
scintillation detection, are also required for APDs: namely, high quantum efficiency, efficient photon ab-
sorption, good response speed and high energy conversion efficiency. Thus, properties mentioned earlier for
common photodiodes also apply to APDs. Quantum efficiencies ranging from 50% to 80%, depending on
the wavelengths of the scintillation photons, are typical for commercial Si APDs. Additionally, gain and
electronic noise properties are important for APD applications. Typical gains exceeding 100 can be achieved;
however, APDs are characteristically noisier than common pn and pin junction photodiodes.
Avalanche Gain
Electron-hole pair production from energetic electrons and holes are usually described by ionization coeffi-
cients α(E) for electrons and β(E) for holes and are the probabilities, per unit differential path-length of travel,
that the charge carrier undergoes an ionizing collision. Typically, for most semiconductors, α(E) > β(E),
although there are exceptions. For instance, in Ge 2α  β, yet for Si α > β and for GaAs α β [Melchior
1972].
Consider a pin APD with a depletion region x ∈ (0, W ) in which a current of holes Ih (x) flows from
holes injected at x = 0, which increases from x = 0 to x = W as a result of impact ionizations. Likewise a
current of electrons Ie (x) is formed that increase from x = W to x = 0. Under steady-state conditions the
total current I = Ih (x) + Ie (x) is constant, as is the electric field so that α and β are constant throughout
the depletion region. In this case the following balance equation holds:
dIh (x)/qe (increase in holes at x) = (Ih /qe )(β dx) + (Ie /qe )(α dx) (no. e-h pairs produced in dx per s),
or, because Ie (x) = I − Ih (x),
dIh (x)
− (β − α)Ih (x) = αI. (14.76)
dx
The solution of this differential equation, subject to the initial condition I = Ih (W ) = Mh Ih (0) or Ih (0) =
I/Mp where Mp is the multiplication factor for holes,
" #
1 α
Ih (x) = I exp((β − α)x) + [1 − exp(−(β − α))x] . (14.77)
Mh β−α
Sze [1981] considered a more general model in which α and β are functions of position in the depletion region
and obtained
$  x     /=  x
x
1     
Ih (x) = I + α(x ) exp − [β(x ) − α(x )] dx dx exp − [β(x ) − α(x )] dx ,
Mh 0 0 0
(14.78)
which reduces to Eq. (14.77) when α and β are constants.
The hole multiplication factor Mh (or rather its inverse) is readily found from Eq. (14.77) by setting
x = W and setting Ih (W ) = I and performing some algebraic manipulations to obtain
1 β
1− = [1 − e−(β−α)W ]. (14.79)
Mh β−α
Because the avalanche breakdown voltage is the voltage at which Mh approaches infinity, the breakdown
condition is found from Eq. (14.79) by setting 1/Mh to zero. This condition can be written as
β
1= [1 − e−(β−α)W ]. (14.80)
β−α
618 Light Collection Devices Chap. 14

If the avalanche process were initiated by electrons injected at x = W , the same breakdown condition
is obtained [Sze 1981]. This is to be expected since breakdown depends only on what is happening in the
depletion region and not on which charge carriers (or primary current) initiate the avalanche. In the limit
as β → α the multiplication factor of Eq. (14.79), which is the APD gain MAP D , has the limiting value
1
MAP D = . (14.81)
1 − αW
Note that as the product αW approaches unity, the gain progresses towards ∞, a generally undesirable
result for the operation of common APDs. This situation is referred to as avalanche breakdown. However,
there is a practical limitation to MAPD , in which series resistance and space charges limit the overall gain.
An empirical formulation for gain in the pre-breakdown region was reported as [Miller 1955],
1
MAPD = n. (14.82)
1 − (VR /VB )
where VB is the breakdown voltage, VR is the reverse bias voltage, and n depends upon the semiconductor
material and device structure. As VR approaches VB , Melchior and Lynch [1966] developed a description for
gain under high light illumination,

1  VB
MAPD = 
n  , (14.83)
1 − (VR − IR/VB ) VR →VB nIR
where IR is the voltage drop due to series resistance. If the gain is defined as the total amplified (avalanche
enhanced) current Iav divided by the total unamplified primary current Ih , then Eq.  (14.83) reduces to [Sze
1981] MAPD = VB /(nIh R) . Thus the amplified photocurrent is Iav = Ih MAPD = Ih VB /(nR) .
Overall, the APD is operated as a linear amplification device, in which the total current, or integrated
charge, is taken to be a linear function of the energy of light absorbed. However, because the quantum
efficiency for scintillation light is less than unity (less than one electron-hole pair per photon), the APD
is actually measuring the number of photons that strike the diode and not the energy absorbed in the
scintillation crystal. As with PMTs, it is assumed that the total number of photons striking the APD is
a linear function of energy absorbed in the scintillation detector. This assumption is mostly true despite
issues with non-linear light output for many scintillators. Hence, the magnitude of the output current gives
a measure of the initial energy absorbed in the scintillation crystal.
APD Designs
Various configurations for avalanche photodiodes have been explored, of which three are shown in Fig. 14.34.
Most commercial APDs are fabricated from Si, although APDs made from commercial low-noise InGaAs and
designed for photon wavelengths between 1.0 and 1.6 μm are also available. The design of Fig. 14.34(a) is
perhaps one of the simplest, relying upon a high electric field at the n+ p junction to produce the avalanching
electric field. The guard ring reduces leakage current and early breakdown at the pn junction corners. The
p+ − π − p − n+ “hi-lo” structure of Fig. 14.34(b) has a similar structure to that of a common IMPATT diode
[Sze 1981]. The p+ π region provides a lower field drift region, in which electrons drift towards the high electric
field region defined at the pn+ junction. The low doped π region allows the active depletion region to extend
nearly completely across the diode. When electrons reach the high field region, an avalanche occurs and
produces the device gain. The beveled sidewalls of the APD design in Fig. 14.34(c) reduce the surface electric
field [Huth et al. 1966], thereby allowing a higher electric field within the semiconductor bulk to promote
avalanche gain. Note that the high field region, defined by the p+ ν junction, is near the thin semiconductor
window. The etched thin window reduces photon absorption losses in the “dead” surface region. Overall,
there are a variety of other APD designs that can be used as sensors for scintillation detectors, some of which
are described elsewhere [Melchior 1972; Sze 1981].
Sec. 14.2. Semiconductor Photodetectors 619

hn hn hn

guard metal contact


ring (n)
SiO2 metal
n+ p+

p+
p p p
n
n+
p+ SiO2 n+

metal contact metal contact


(a) (b) (c)
Figure 14.34. Avalanche photodiodes of three different designs: (a) a Si guard ring
structure avalanche photodiode, (b) a p+ − π − p − n+ avalanche photodiode, and (c) a
deep etched depletion avalanche photodiode with beveled sides.

Noise Factor
Ultimately, the desired feature of any photon detector is a proportional response to the total energy absorbed
in the scintillation crystal attached to the detector. Hence, charge collected from an APD should be a linear
measure of energy deposited in the scintillator, with an energy resolution defined by the variance of the
output signal. Variations in the gain broaden the energy resolution of the scintillation light, and a non-linear
output can make the energy calibration of the pulse height spectra difficult.
As developed in Sec. 10.5.4 for proportional counters, the avalanche process in an APD is statistical in
nature. In other words, the amount of avalanching, and thus gain, for each electron is different, slight as
it may be. Hence, the square of the average gain is not equal to the average gain squared but, rather the
variance in the gain is
σM2
= M 2  − M 2 . (14.84)
The “noise factor” is defined as
M 2 
F = . (14.85)
M 2
From Eqs. (14.84) and (14.85), the variance in the gain is
2
σM = (F − 1)M 2 . (14.86)

Note that if the gain variance is zero, then F = 1.


The mean square shot noise current for a reverse biased pn junction is defined as

i2  = 2qe IB, (14.87)

where B is the bandwidth in Hz. If a uniform avalanche multiplication region exists, the differential mean
square shot noise di2  for the differential current dI generated within element dx at x is multiplied by the
mean square gain at x, M 2 (x), to yield

di2 
dφ(x) = = 2qe d I(x)M (x)2 , (14.88)
B
620 Light Collection Devices Chap. 14

Figure 14.35. Noise factor as a function of gain M and the ratio α/β.

where φ is termed the “spectral density,” and Eq. (14.87) represents a portion of the total mean square noise
current. Integration of Eq. (14.87) yields the total noise contribution of the multiplication process. If β = kα
(or k −1 = α/β), where k is a scaling constant, and M is independent of x, McIntyre [1966] shows that the
noise factors for electron and hole injection are
  2    2 
φ M −1 φ (1 − k) M − 1
Fe = = M 1 − (1 − k) and Fh = =M 1+ .
2qe IM 2 M 2qe IM 2 k M
(14.89)
The results from Eqs. 14.89 for several M and α/β are plotted in Fig. 14.35. In the case that α = β, or
k = 1, then both Eqs. 14.89 reduce to F = M . For the case of electron injection, in which holes play no
part in the avalanche process (β = 0), Eq. (14.89) reduces to,
 
2M − 1
Fe = . (14.90)
M

This result reduces to Fe  2 as M → ∞. A similar result is achieved if holes play the major part in the
avalanche current and electrons do not contribute to the avalanche.15

15 Hence, k −1 → 0, as shown in Fig. 14.35.


Sec. 14.2. Semiconductor Photodetectors 621

14.2.4 Semiconductor Photomultipliers


Junction breakdown of semiconductors can be used as another means of radiation counting and spectroscopy.
For any pn junction operated with a reverse bias voltage, there is a voltage above which the junction “breaks
down” and continues to conduct current across the semiconductor. This phenomenon is initiated by three
different means, namely (1) thermal instabilities, (2) tunneling current, and (3) avalanche breakdown.
Here it is avalanche breakdown that is of interest. Avalanche breakdown occurs when Eq. (14.78) is
W
satisfied. Should α = β, then the breakdown condition is achieved when 0 α(x) dx = 1. The critical
electric field required to sustain the avalanche condition is EA = 2VB /W , where VB is the breakdown voltage
[Sze 1981].
The avalanche process is solely dependent upon what occurs within the depletion region W . Hence, an
event that excites a charge carrier within the active depletion region may trigger an enormous, continuous
avalanche from impact ionization with gains exceeding 106 . This interesting mode of operation is usually
not preferred for APD operation, the effects of which were studied by McIntyre [1961] and Haitz [1961].
However, there are particular applications in which the breakdown mode of operation is beneficial, mainly
realized with the single-photon avalanche diode (SPAD), so-named because of its ability to detect low light
levels, one photon at a time. The leading edge of an avalanche signal marks the arrival time of the interacting
photon within the depletion region, and SPADs with 28 ps timing resolution at room temperature have been
reported [Cova et al. 1989]. After the avalanche is triggered, the self-sustained current continues to flow unless
quenched. Often a series resistance is included in the design that serves to quench the avalanche, much like
an externally quenched GM counter. As a matter of fact, APDs designed and operated in this mode are
often said to operate in “Geiger Mode” [Renker 2006]. As the avalanche current flows through the quenching
resistance, it draws voltage from the source, thereby causing the voltage across the APD to drop below the
breakdown voltage, causing the avalanche to cease. As a result, the output current and collected charge
are nearly the same for each avalanche regardless of energy deposition in the device, statistical fluctuations
notwithstanding. Consequently, if two or more photons interact in the device simultaneously, the total charge
liberated from the quenched avalanche is roughly the same as if a single photon caused the avalanche, again
much like a GM counter.
Silicon photomultipliers (SiPM)16 use the breakdown condition with thousands of tiny silicon APDs
arranged into a compact array, presently on the order of 6 mm × 6 mm area or less. The individual APDs
in silicon photomultipliers (SiPM) have linear dimensions usually between 20 μm and 100 μm, a common
size is 35 μm × 35 μm per APD pixel. Hence a single SiPM array may have more than 104 APD pixels.
Each APD is electrically decoupled from adjacent APDs with polysilicon resistors fabricated on the same
substrate. Typical operational bias voltage is 10% to 15% above the breakdown voltage. A scintillator may
be fastened to the SiPM face, much like a conventional PMT, and light from radiation interactions within
the scintillator triggers the APDs. Each APD provides information that is ultimately limited to recognizing
the excitation of an electron-hole pair within the avalanche region. Because each pixel produces an avalanche
of relatively the same magnitude per event, the total photon count can be determined by dividing the total
measured charge by the avalanche gain. Hence, the device operates mainly as a photon counter, and the
total measured current is proportional to the total number of photons. The enormous gain per pixel, when
the pixel counts are added together, can produce more than 109 free electrons per event. Properties of
commercially available SiPMs are given in Table 14.9.
General SiPM Characteristics
A particular advantage of SiPMs is the high quantum efficiency of Si for photons with wavelengths between
350 nm and 950 nm. The increased probability of absorption of scintillation photons, in the active volume of

16 Also called multi-pixel photon counters (MPPC).


622 Light Collection Devices Chap. 14

Table 14.9. Properties of some commercial silicon photomultipliers. The legend abbreviations are as follows: A
manufacturer (H Hamamatsu, K Ketek, S SensL); B model; C SiPM chip size (x mm × x mm); D microcell pixel size
(x μm × x μm); E number of microcells; F microcell fill factor (%); G gain at room temperature ×106 ; H breakdown
voltage, VBr (volts); I bias range above VBr (volts); J peak wavelength (nm); K maximum photon detection efficiency
(%) at peak wavelength and max voltage; L dark count rate (kHz); M signal rise time (ns); N signal pulse width
(FWHM in ns); O microcell recovery time (ns); P VBr temperature drift (mV/◦ C); and Q gain drift (%/◦ C). Non-
reported table entries are indicated by NR.

A B C D E F G H I J K L M N O P Q

S 10010B 1 10 2880 28 0.2 24.5 ± 0.5 1-5 420 18 700 0.3 0.7 10 21.5 -0.8
S 10020B 1 20 1296 48 1 24.5 ± 0.5 1-5 420 31 700 0.3 0.7 50 21.5 -0.8
S 10035B 1 35 576 64 3 24.5 ± 0.5 1-5 420 41 700 0.3 0.7 180 21.5 -0.8
S 10050B 1 50 324 72 6 24.5 ± 0.5 1-5 420 47 800 0.3 0.7 350 21.5 -0.8
S 30020B 3 20 10998 48 1 24.5 ± 0.5 1-5 420 31 6600 0.6 1.3 100 21.5 -0.8
S 30035B 3 35 4774 64 3 24.5 ± 0.5 1-5 420 41 6700 0.6 1.3 180 21.5 -0.8
S 30050B 3 50 2668 72 6 24.5 ± 0.5 1-5 420 47 7500 0.6 1.3 350 21.5 -0.8
S 60035B 6 35 18980 64 3 24.5 ± 0.5 1-5 420 41 21500 1 3.2 210 21.5 -0.8
S 10010C 1 10 2880 28 2 24.65 ± 0.25 1-5 420 41 30 0.3 0.6 10 21.5 -0.8
S 10020C 1 20 1296 48 1 24.65 ± 0.25 1-5 420 41 30 0.3 0.6 90 21.5 -0.8
S 10035C 1 35 576 64 3 24.65 ± 0.25 1-5 420 41 30 0.3 0.6 180 21.5 -0.8
S 10050C 1 50 324 72 6 24.65 ± 0.25 1-5 420 41 30 0.3 0.6 350 21.5 -0.8
S 30020C 3 20 10998 48 1 24.65 ± 0.25 1-5 420 41 300 0.6 1.5 90 21.5 -0.8
S 30035C 3 35 4774 64 3 24.65 ± 0.25 1-5 420 41 300 0.6 1.5 180 21.5 -0.8
S 30050C 3 50 2668 72 6 24.65 ± 0.25 1-5 420 47 300 0.6 1.5 350 21.5 -0.8
S 60035C 6 35 18980 64 3 24.65 ± 0.25 1-5 420 41 1200 1 3.2 210 21.5 -0.8
H S12571-010 1 NR 10000 33 0.135 65 ± 10 4.5 470 10 100 NR 0.3 NR 60 1.2
H S12571-015 1 NR 4489 53 0.23 65 ± 10 4 460 25 100 NR 0.25 NR 60 1.5
H S12571-025 1 NR 1600 65 0.515 65 ± 10 3.5 450 35 100 NR 0.25 NR 60 1.6
H S12571-050 1 NR 400 62 1.25 65 ± 10 2.6 450 35 100 NR 0.25 NR 60 2.16
H S12571-100 1 NR 100 78 2.8 65 ± 10 1.4 450 35 100 NR 0.3 NR 60 4.3
H S12572-010 3 NR 90000 33 0.135 65 ± 10 4.5 470 10 1000 NR 0.3 NR 60 1.2
H S12572-015 1 NR 40000 53 0.23 65 ± 10 4 460 25 1000 NR 0.25 NR 60 1.5
H S12572-025 1 NR 14400 65 0.515 65 ± 10 3.5 450 35 1000 NR 0.25 NR 60 1.6
H S12572-050 1 NR 3600 62 1.25 65 ± 10 2.6 450 35 1000 NR 0.25 NR 60 2.16
H S12572-100 1 NR 900 78 2.8 65 ± 10 1.4 450 35 1000 NR 0.3 NR 60 4.3
H S12576-050 1 NR 400 NR 1.25 62.9 ± 10 2.6 450 35 5 NR 0.25 NR 60 2.16
H S12577-050 3 NR 3600 NR 1.25 62.9 ± 10 2.6 450 35 50 NR 0.25 NR 60 2.16
K PM1150 1.2 50 576 70 1.7 25 ± 3 2.5-5 420 > 50 < 400 NR NR NR NR <1
K PM1150T 1.2 50 576 63 8 25 ± 3 2.5-5 420 > 50 < 400 NR NR NR NR <1
K PM3350 3 50 3600 70 8 25 ± 3 2.5-5 420 > 50 < 500 NR NR NR NR <1
K PM3350T 3 50 3600 63 6 25 ± 3 2.5-5 420 > 40 < 500 NR NR NR NR <1
K PM6660 6 60 10000 66 10 24 2.4-4.8 420 > 50 < 500 NR NR NR NR <1

the APD, is a clear advantage of the SiPM when compared to the smaller absorption probabilities in PMT
semitransparent photocathodes or PMT reflective photocathodes. Hence, the photon detection efficiency of
a SiPM can be much higher than that of a common PMT. However, many commercial SiPM units usually
have a peak sensitivity near 420 nm, much like that of conventional bialkali PMTs. SiPMs are compact
and rugged, which allows them to be fabricated as compact instruments and dosimeters. This compactness
is perhaps one of the most useful features of SiPMs compared to vacuum tube PMTs. Further, they need
only modest power, usually requiring no more than a few tens of volts for operation, which is substantially
less than that needed for a PMT. SiPMs are also insensitive to magnetic fields, thereby making them an
attractive choice for applications in areas where high magnetic fields may arise. Typically, the total array of
APDs in the SiPM has an extremely fast rise time, between 0.3 and 1 ns. However, the actual recovery time
Sec. 14.2. Semiconductor Photodetectors 623

required for the SiPM is much longer and usually ranges from a few tens of ns up to 400 ns, depending on
the pixel and array sizes. Hence, the rise times and count rates are comparable to conventional PMTs.
Presently the cost of a single SiPM array chip is modest, yet these devices range in area from only 1 mm
× 1 mm up to 6 mm × 6 mm. Such small light detectors might be adequate for small projects and compact
scintillation applications. However, to cover the same area as a 3-inch diameter bialkali PMT, typically used
for scintillation spectroscopy, a minimum of 127 SiPM chips are needed, if the larger 6 mm × 6 mm chips
are used. Commercially available SiPM arrays are available, presently with a maximum size of 6 mm × 6
mm chips arranged in an 8 × 8 array that has the equivalent area of a two-inch diameter PMT. At the time
of writing, the cost of such an array is considerably higher than the PMT counterpart. However, commercial
scintillation detector units have recently become available with a SiPM readout option.
Unlike a PMT photocathode, SiPMs have regions between the diodes that are insensitive to illumination.
The ratio of the sensitive area to the total area is termed the “fill factor.” Modern commercial units have
fill factors ranging between about 30% to 70%. As fill factor increases, the possibility of cross talk between
pixels also increases. Cross talk may manifest itself as photon emissions from de-exited electrons, and their
subsequent absorption in adjacent pixel cells. Hence, a photon emitted in one pixel cell can trigger an
avalanche in an adjacent cell. One method proposed to reduce this effect is the incorporation of etched
trenches between the pixels. The trenches are then backfilled with an opaque material [Piemonte 2006].
However, if de-excitation photons are emitted from a pixel cell and towards the scintillator, it is also possible
that they are subsequently reflected into a different pixel cell, thereby triggering an unwanted avalanche.
Cross talk for commercial SiPMs ranges between < 1% to 35% and generally increases with the sizes of pixel
cell and the array.
Another minor problem with APDs is the possibility of stray avalanches arising from the emission of
charge carriers from trapping sites, an effect referred to as “afterpulsing”. Electrons and holes flowing in the
APD can become trapped in impurity and defect centers and are later emitted from the traps with a time
constant, which strongly depends on the energy level of the trap. Whenever they are emitted, the detrapping
of these charge carriers can trigger another avalanche, which may be included in the overall measurement
of the initial scintillation event, thereby overestimating the light yield. Afterpulsing for commercial SiPMs
ranges between 0.2% and 0.6%.
It is also possible that more than one photon strikes a pixel simultaneously (or at least within the
pixel recovery time), so that only one of the photons is recorded. The compact pixel arrays are designed
such that simultaneous interactions are relatively improbable, usually with negligible effect on performance.
However, as the total light fluence from a scintillation event increases, and the decay time of the scintillator
decreases, the probability of nearly simultaneous absorptions increases. Consequently, the measured current
underestimates the measured light, producing non-linearity in the output spectrum. As the light intensity
increases, the SiPM output becomes increasingly disproportionate to the number of scintillation photons
produced.
A breakdown avalanche can also be triggered by thermally generated charge carriers and thus can cause
problematic background count rates. The dark current, and count rate, from thermal excitation can be
relatively large, ranging from 3 × 104 cps to 3 × 106 cps for commercial units and increases with pixel size
and SiPM array size. This problem can be greatly mitigated by operating the device at reduced temperatures.
Further, randomly triggered events ultimately produce an avalanche from a single pixel, which produces a
substantially lower current than expected from a scintillation flash. Unless the device is being operated as
a single photon detector for a low level light source, the use of a discriminator set at a reasonable threshold
helps defeat this problem.
624 Light Collection Devices Chap. 14

PROBLEMS
1. A NaI(Tl) crystal is coupled to a PMT having a Corning 7044 borosilicate window. The coupling
compound Dow-Corning Q2-3067 has an index of refraction of 1.48. At the peak wavelength, determine
the critical angle in the NaI(Tl) crystal for light passing through to the photocathode layer in the PMT.

2. Determine the value of τ (λ) for borosilicate glass and LiF at the wavelengths of 300 nm and 400 nm.

3. If there are no window absorption losses and the reflectance R(λ) is small, show from Eqs. (14.10) and
(14.11) that the total transmittance for a glass PMT window is described by

(1 − R(λ))2 2n(λ)
T (λ) =  .
1 − R2 (λ) n(λ)2 + 1

where one interface is surrounded by air and the other interface is at vacuum.

4. Determine the free electron concentration for Li, Na, K, Rb and Cs at absolute zero.

5. Determine the thermionic emission current density for a S-11 response PMT at a temperature of 32◦ C
and compare it to that of a S-24 response PMT.

6. Determine the electron cutoff energy for the peak wavelength emission from a LaBr3 detector coupled
to a pure CsSb3 photocathode. Repeat for a Na2 KSb photocathode.

7. Show that Eq. (14.37) can be cast into the form Eq. (14.38). Hint: Start with the substitution y(x) ≡
E(x).

8. Given a 10-stage PMT with α = 0.72 and a gain of 106 at 700 volts, find the value of k. What is the
new gain if the voltage is increased to 800 volts?

9. The dark current from a PMT with an electron gain of 5 × 105 is measured to be 1.5 mA. What is the
corresponding emission rate of electrons from the photodiode?

10. A LaBr3 :Ce detector is coupled to a PMT having a KCs photocathode in a borosilicate envelope. The
detector is being used to detect gamma rays from a 137 Cs source. With 90% light impinging on the
glass interface at all angles, determine the output charge from full energy absorption with a 10-stage
PMT having the following properties: ηi = 0.98, ηa = 0.98, δi = 4 for the first 5 stages, and δi = 3.8 for
the last five stages.

11. What are the advantages of using a microchannel PM tube compared to one of conventional design?

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17 Interestingly,
there is no “Part I” by G.A. Morton. In the beginning of the article, Morton mentions this paper as being added
to the story written by R.A. Hofstadter which was published directly before this work in IEEE Trans. Nucl. Sci., NS-22,
13–25, (1975a). Hence, this reference is “Part II” to the story begun by Hofstadter.
Chapter 15

Basics of Semiconductor
Detector Devices

It has today occurred to me that an amplifier using semiconductors


rather than vacuum is in principle possible.
William Shockley

15.1 Introduction
Semiconductors are much better for energy spectroscopy than are gas-filled or scintillation detectors because
semiconductors have vastly superior energy resolution. This improved resolution is largely due to the better
statistics caused by the larger numbers of signal carriers (charges) produced by a radiation interaction.
On average, it takes only 3 to 5 eV to produce an electron-hole pair in a semiconductor. By comparison,
it takes between 25 and 40 eV to produce an electron-ion pair in a gas-filled detector and between 100
eV and 1 keV to produce a single photoelectron ejection from the photocathode of a photomultiplier tube
(PMT) in a scintillation/PMT detector, a consequence of light reflections and poor quantum efficiency at
the photocathode. Hence, a semiconductor produces considerably more charge carriers from the primary
ionization event and, thereby reduces the statistical fluctuations in the energy resolution.
Semiconductor radiation detectors have many different shapes, sizes, and configurations, yet there are
some basic designs that, in some form or another, can be attributed to practically all semiconductor radiation
detectors. These basic designs include pn-junction diodes, pin-junction diodes, Schottky diodes, resistive
detectors, and photoconductors. The vast field of semiconductor device physics is much too large to describe
in a single book chapter. As a result, only those concepts needed to understand basic detector operations
and characteristics are offered here.
The general purpose of this text is to familiarize the reader with various aspects of radiation detectors
so that the skills to design, fabricate, characterize, and deploy such devices are acquired. Proficiency in
detector design and fabrication requires an understanding of basic solid state and semiconductor physics,
hence the reason for the preceding and present chapters. In this chapter, the basic physics used to make
semiconductors into radiation detectors is summarized. In this chapter much of the notation introduced
in Chapter 12 is used extensively without any further explanation. Finally, values of the many physical
constants used here and in other chapters are tabulated in Appendix A.

15.2 Charge Carrier Collection


Charge carriers in the conduction band spontaneously drop back into empty states in the valence band, while,
at the same time, other electrons gain energy to cross the band gap. Overall, a somewhat constant density
of electrons and holes remains in the conduction and valence bands, respectively. The time over which a
charge carrier remains in either band is altered by impurity and defect states that appear in the band gap.

627
628 Basics of Semiconductor Detector Devices Chap. 15

These traps and defects increase the probability of electrons or holes moving from either band edge to an
intermediate state before completing the recombination process. If a charge carrier falls into a defect state,
it is referred to as “trapped”; whereas, if the charge carrier’s journey is completed, e.g., an electron falls
completely back into a hole in the valence band, it is referred to as having “recombined”. The average time
over which an excited electron remains in the conduction band before being trapped or recombining is the
electron lifetime τe . Similarly, the average time in which a hole remains in the valence band before being
trapped or recombining is the hole lifetime τh .

15.2.1 Charge Carrier Generation, Recombination and Injection


The concentration of charge carriers in the conduction and valence bands of a semiconductor is temperature
dependent. As the population of electrons and holes increases, the probability that electrons return to the
valence band and recombine with holes also increases. The overall process reaches a thermal equilibrium, in
which np = n2i .
Other sources of energy deposition, such as the photoelectric effect,
EC can excite charge carriers from the valence band into the conduction
band (see Fig. 15.1). The introduction of these extra charge carriers is
commonly referred to as charge carrier injection, and produces a non-
Gph Gth R equilibrium condition in the semiconductor. The continuous constant
injection of charge may reach a steady-state, but the semiconductor
EV cannot reach its equilibrium until the source of the charge injection
is stopped. Semiconductor radiation detectors rely upon the charge
Figure 15.1. Thermal generation Gth , injection process to excite electron-hole pairs, in which the deposition
photo-generation Gph , and recombina-
tion R of electron-hole pairs across the of radiation energy in the semiconductor produce excess electron and
band gap of a semiconductor. hole populations, Δn and Δp, thereby producing the condition np >
n2i . These excess charge carriers can be measured to indicate the
presence, and often energy, of the radiation particles interacting in the semiconductor.

15.2.2 Radiative Recombination


Consider a semiconductor material, initially at equilibrium, that has a package of charge Δn injected into
the bulk material. Because these charges are excited from the valence band, an equal package of excess holes
Δp appears in the valence band. Let the recombination rate with an excess of electrons be rn (n, p) and the
equilibrium recombination rate be rn (no , po ), in which the notation no and po are used for the equilibrium
electron and hole concentrations. The change in electron recombination rate from the equilibrium case after
charge injection is
Rn = rn (n, p) − rn (no , po ). (15.1)
Likewise, for hole recombination,
Rp = rp (n, p) − rp (no , po ). (15.2)
The electron lifetime is defined as the excess electron concentration divided by the change in recombination
rate, i.e.,
n − no Δn
τn = = (15.3)
Rn Rn
and the hole lifetime is
p − po Δp
τp = = . (15.4)
Rp Rp
Radiative electron recombination refers to a direct transition from the conduction band to the valence
band, during which a photon is released by the de-excitation of the electron. This process can occur only
Sec. 15.2. Charge Carrier Collection 629

if a hole is available to complete the recombination process. Hence, the recombination rate is proportional
to the product of electron and hole concentrations, i.e., rn = rp = βnp, where β is an empirical, radiative-
recombination, proportionality constant. From Eq. (15.1), the change in electron recombination after carrier
injection becomes
Rn = Rp = β(np − n2i ). (15.5)

Because Δn = Δp, τn must equal τp . Substitution of Eq. (15.5) into Eq. (15.3) yields

n − no Δn 1
τn = τp = = = . (15.6)
β(np − n2i ) β([no + Δn][po + Δn] − n2i ) β(no + po + Δn)

Here the equilibrium condition no po = n2i has been invoked. This result shows that radiative recombination
is inversely proportional, in all circumstances, to the total concentration of charge carriers.

15.2.3 Shockley-Read-Hall Recombination


Material imperfections often introduce energy states or traps
EC in the band gap that, in turn, can participate in the recombi-
electron electron
emission trapping
nation process. Typically, this trap-assisted recombination,
known as Shockley-Read-Hall (SRH) recombination, is more
likely to occur than are direct radiative transitions (see ar-
guments in Shockley and Read [1952], Hall [1952, 1959] and
hole hole Varshni [1967]). The processes of SRH trapping are illus-
emission trapping trated in Fig. 15.2.
EV Consider a concentration of imperfections in a semicon-
ductor with trapping states at energy ET . These trapping
Figure 15.2. Shockley-Read-Hall recombination de- sites may arise from native defects, such as anti-sites, voids
picting electrons and holes emitted and trapped in en- and interstitials, or may result from impurities in the ma-
ergy states arising from material imperfections.
terial. The probability that an electron is captured by an
electron trap at energy ET is a function of the unfilled trap density NT and the electron population n, with
capture rate
nβcn NT
Rcn = nβcn NT [1 − fF D (ET )] = , (15.7)
EF − ET
1 + exp
kT
where βcn is a proportionality constant for electron capture. For those traps that are occupied by an electron,
the rate at which electrons are emitted into the conduction band is

βen NT
Ren = βen NT fF D (ET ) = , (15.8)
ET − EF
1 + exp
kT

where βen is a proportionality constant for electron emission.


At equilibrium, the rate at which electrons arrive in the conduction band must be equal to the rate at
which they are captured from the conduction band, i.e.,

[1 − fF D (ET )] ET − EF
βen = βcn no = βcn no exp . (15.9)
fF D (ET ) kT
630 Basics of Semiconductor Detector Devices Chap. 15

where no is the equilibrium electron concentration. For a non-degenerate semiconductor, no is described by


Eq. (12.126), which when substituted into Eq. (15.9) gives

ET − EC
βen = βcn NC exp . (15.10)
kT

In the case that the trap energy ET is equal to EF

EF − EC
βen = βcn NC exp = βcn n1 , (15.11)
kT

where n1 is the electron concentration in the conduction band if EF = ET . The net rate Rn at which
electrons are captured from the conduction band is the difference between Eq. (15.7) and Eq. (15.8), so that
with Eq. (15.10) one obtains

Rn = Rcn − Ren = βcn NT {n[1 − fF D (ET )] − n1 fF D (ET )}. (15.12)

In the same manner used above for electrons, the rate at which holes are captured from the valence band
into traps or, equivalently the rate at which traps are filled with electrons is
pβcp NT
Rcp = pβcp NT fF D (ET ) = , (15.13)
ET − EF
1 + exp
kT

where βcp is the proportionality constant for hole capture. The rate at which holes are emitted from the
trap as electrons move from the valence band into the traps is
βep NT
Rep = βep NT [1 − fF D (ET )] = , (15.14)
EF − ET
1 + exp
kT

where βep is the proportionality constant for hole emission. Making the emission and capture rates equal
yields,
fF D (ET ) EF − ET
βep = βcp po = βcp po exp . (15.15)
[1 − fF D (ET )] kT
At equilibrium, the hole capture and emission rates must be equal and the hole concentration in the con-
duction band is po . Substitution of Eq. (12.128) for po into Eq. (15.15), the emission rate for holes is found
to be
EV − ET
βep = βcp NV exp . (15.16)
kT
If the trap energy ET is equal to EF

EV − EF
βep = βcp NV exp = βcp p1 . (15.17)
kT

where p1 is the hole concentration in the valence band at EF = ET . The net rate at which holes are captured
from the valence band is the difference between Eq. (15.13) and Eq. (15.14), and with βep = βcp p1 from
Eq. (15.17),
Rp = Rcp − Rep = βcp NT {pfF D (ET ) − p1 [1 − fF D (ET )]}. (15.18)
Sec. 15.2. Charge Carrier Collection 631

Unlike pure radiative recombination, with carrier injection, it is quite possible that Δn = Δp, mainly
because the carrier capture coefficients for electrons and holes may be quite different. This issue becomes
more important as the trap density in a semiconductor increases. For the following derivation, however, it
is assumed that the trap density is relatively low so that, even in the non-equilibrium condition, Δn  Δp.
Hence, Eq. (15.12) and Eq. (15.18) are equal. Equating the right-hand sides of Eq. (15.12) and Eq. (15.18)
and solving for fF D (ET ) one obtains
βcp p1 + βcn n
fF D (ET ) = . (15.19)
βcn (n + n1 ) + βcp (p + p1 )
Substitute this result into either Eq. (15.12) or Eq. (15.18) to find
βcn βcp NT (pn − n2i )
Rn = Rp = , (15.20)
βcn (n + n1 ) + βcp (p + p1 )
in which it is recognized that n1 p1 = n2i . Division of the numerator and denominator of Eq. (15.20) by
βcn βce NT gives
pn − n2i
Rn = Rp = . (15.21)
1 1
(n + n1 ) + (p + p1 )
βcp NT βcn NT
Finally, define the trapping time for electrons as τn = 1/(βcn NT ) and the trapping time for holes as
τp = 1/(βcp NT ), and substitute these definitions into Eq. (15.22) to obtain the general expression for SRH
recombination rates, namely

pn − n2i
Rn = Rp = . (15.22)
τp (n + n1 ) + τn (p + p1 )

Note that at equilibrium np = n2i and Eq. (15.22) at the net recombination rate is zero.

15.2.4 Equations of Continuity


In a semiconductor, even in non-steady-state conditions, the hole generation rate must always equal the
electron generation rate, i.e., gn = gp . Similarly, the hole and electron recombination rates must always be
equal, i.e., n/τn = p/τp . The generation rates, carrier concentrations and lifetimes are, generally, functions
of position r in the crystal and time.
In this section the continuity equations that determine the free electron concentration n(r, t) and the
hole concentration p(r, t) are developed. Begin by first considering the free electrons in a small but arbitrary
volume V of a semiconductor. In this volume, the following balance relation must apply:
⎧ ⎫
⎧ ⎫ rate at which ⎪
the net ⎪ ⎧ ⎫ ⎧ ⎫ ⎪ ⎪ ⎪


⎪ ⎪
⎪ ⎪ generation⎪ ⎪rate of recom-⎪ ⎪ ⎪
⎪ free electrons ⎪


⎨rate of ⎬ ⎨ ⎬ ⎨ ⎬ ⎨ ⎬
rate in V bination of flow out of V
increase in = − − . (15.23)

⎪ ⎪
⎪ ⎪
⎩ of free ⎪
⎭ ⎪
⎩ electrons with ⎪
⎭ ⎪
⎪ through the ⎪ ⎪

⎩V of free ⎭ ⎪ ⎪
⎪ ⎪

electrons
electrons holes in V ⎩surrounding ⎪
⎪ ⎭
surface S
In symbols, this balance relation is written as
   
∂n n
dV = dV gn − dV − dS Jn •n̂, (15.24)
V ∂t V V τn S
632 Basics of Semiconductor Detector Devices Chap. 15

where dS is a differential element of the surface with outward normal n̂ and Jn (r, t) is the current vector,
i.e., the flow rate of free electrons across a unit area perpendicular to Jn .
The last term in Eq. (15.24) can be written as a volume integral by use of Gauss’s theorem, namely
 
dS Jn n̂ =
• dV ∇•Jn . (15.25)
S V

With this result, all the terms in Eq. (15.24) can be combined into a single integral, namely
 " #
∂n n
dV − gn + + ∇ Jn = 0.
• (15.26)
V ∂t τn
But V is arbitrary, and the only integrand that integrates to zero for arbitrary integration limits is the zero
integrand. Hence the balance condition is
∂n n
= −∇•Jn + gn − . (15.27)
∂t τn
A similar derivation can be made to derive a balance relation for the hole concentration p(r, t). The
result is
∂p p
= −∇•Jp + gp − . (15.28)
∂t τn
Equations (15.27) and (15.28) are often referred to as the continuity equations.
Before these equations can be used to find n(r, t) and p(r, t), the hole and electron current vectors must
be written in terms of the concentrations. This can be done by writing Jn and Jp as a sum of a current from
a diffusion process and a drift current caused by an electric field E.1 In the diffusion process, charge carriers
are assumed to flow away from regions of higher concentration according to Fick’s law.2 The currents of the
free electrons and holes are written as

Jn = −Dn ∇n − nμn E, (15.29)

Jp = −Dp ∇p + pμp E, (15.30)

where μn is the electron mobility and μp is the hole mobility. The diffusion coefficients can be evaluated in
terms of mobilities as [McKelvey 1966]
μn kT μp kT
Dn = and Dp = , (15.31)
qe qe
which are often called the Einstein relationships.
Substitution of Eqs. (15.29) and (15.30) into Eqs. (15.27) and (15.28) gives
∂n n
= Dn ∇2 n + μn ∇•(nE) + gn − , (15.32)
∂t τn
∂p p
= Dp ∇2 p − μp ∇•(pE) + gp − . (15.33)
∂t τp

1 Itis assumed here that there are negligible magnetic fields.


2 This is analogous to Fourier’s law of heat conduction, in which heat energy flows away from regions at higher temperature into
regions of lower temperature. Thus, free electrons flow, as a result of their random thermal motion, in the opposite direction
of the electron density’s greatest rate of increase, i.e., Jn = −Dn ∇n, where Dn is the diffusion coefficient.
Sec. 15.2. Charge Carrier Collection 633

The drift terms in these continuity equations can be put into a more tractable form by use of the vector
identity
∇•(nE) = E •∇n + n∇•E. (15.34)
Finally, it is convenient to express the generation rate (gn or gp ) as the sum of the thermal generation rate
(gon or gop ) plus the rate at which the carriers are produced in excess of the thermal generation rate (gn or
gp ), i.e.,
gn = gon + gn and gp = gop + gp . (15.35)
With these alterations, the continuity equations assume the form

 
∂n n no
= Dn ∇2 n + μn (E •∇n + n∇•E) + gn − −
∂t τn τn
(15.36)
 
∂p p po
= Dp ∇2 p − μp (E •∇p + p∇•E) + gp − −
∂t τp τp

An Example of the Use of the Continuity Equation: Consider the case in which charge is injected,
continuously at a constant rate, into the end of a semiconductor block without an electric field present,
as depicted in Fig. 15.3. Eventually, the distribution of free electrons assumes a steady-state distribution
along the length of the semiconductor. The one-dimensional, steady-state form of Eq. (15.36), with E = 0,
gives the following equation for the right-hand portion of the semiconductor in which no charge is injected
(gn = 0).
d2 n(x) n(x) − no
Dn − = 0. (15.37)
dx2 τn
The general solution for n(x) − no is

x −x
n(x) − no = Δn(x) = C1 exp √ + C2 exp √ , (15.38)
Dn τn Dn τn

where C1 and C2 are arbitrary constants and Dn τn is the electron diffusion length Ln . Application of the
boundary conditions that as x → ∞ n(x, t) must remain finite implies C1 must be zero. So in the right-hand
portion of the semiconductor the electron density must vary as

−x
n(x) = no + C2 exp √ , (15.39)
Dn τn
where C2 depends on n(x) in the injection region. At the location x = 0, the injected charge is Δn, so that

−x
n(x) = no + Δn exp √ , (15.40)
Dn τn
from which the injected electron population is seen to exponentially decrease with x.
In a similar fashion, if holes are injected into the left-hand end of the semiconductor. The steady-state
hole density p(x) in the right portion of the semiconductor where there is no charge injection is the solution
of
d2 p(x) p(x) − po
Dp − = 0. (15.41)
dx2 τp
634 Basics of Semiconductor Detector Devices Chap. 15

photons
E > Eg

injected
e-h pairs
semiconductor

n
é -x ù
n0 + Dn exp ê ú
êë Dnt n úû

n0
x

Figure 15.3. Electron-hole pairs can be injected through the photoelectric ef-
fect. Their population decreases through recombination as they diffuse through
the semiconductor.

The general solution for p(x) − po is


   
x −x
p − po = Δp(x) = C3 exp  + C4 exp  , (15.42)
Dp τp Dp τp

where again C3 and C4 are arbitrary constants and Dp τp is the hole diffusion length Lp . Because p must
remain finite as x → ∞, C3 must vanish so the solution to the present problem is
 
−x
p(x) = po + C4 exp  . (15.43)
Dp τp
At the location x = 0, the injected charge is Δp so the above result becomes
−x
p(x) = po + Δp exp √ , (15.44)
Dn τn
from which the injected hole population is seen to exponentially decrease with increasing x.

15.3 Basic Semiconductor Detector Configurations


Semiconductor detectors can be fashioned into many different configurations, including junction diodes,
Schottky barrier diodes, photoconductors, and photoresistors. To select the most appropriate configuration,
Sec. 15.3. Basic Semiconductor Detector Configurations 635

one must consider the semiconductor material and the radiation detection application. Some semiconductor
materials are composed of substances that are not easily converted into junction diodes, such as HgI2 and
PbI2 , whereas other semiconductors, such as Si and Ge, are easily fashioned into junction devices. Some
materials, such as GaAs, can be fabricated easily into either photoconductors or Schottky barrier devices.
Limited doping selection and other chemical constraints prevent some materials to be configured easily
as either reverse biased diodes or photoconductors. The following section introduces the reader to basic
semiconductor configurations.

15.3.1 The pn Junction


If two blocks of semiconductor material, one doped with concentration ND donors and the other doped with
concentration NA acceptors, are brought into contact, then the p-type side of the junction boundary has an
excess of free hole charge carriers and the n-type side of the junction has an excess of free electron charge
carriers (see Fig. 15.4). The concentration gradient across the junction boundary causes holes to diffuse
across the boundary into the n-type side, and electrons to diffuse to the p-type side (see Fig. 15.5). The free
carriers leave behind the immobile host ions, which produce a region of space charge of opposite polarity,
as depicted in Fig. 15.6. The result is the production of an internal electric field with an applied force in
the opposite direction of the diffusion current. The presence of space charge distorts the band energy levels
and causes the bands to bend across the junction boundary. The bands distort and bend until the diffusion
current is equal to the electric-field current, thereby producing a state of equilibrium. In other words, the
concentration gradient force that causes diffusion current matches the electric field force that causes the drift
current in the opposite direction, such that a state of equilibrium is reached, as depicted in Fig. 15.6.

stationary stationary
- acceptor ion + donor ion

+ hole - electron

stationary stationary - - - + + +
- acceptor ion + donor ion + + +
- -
- - - - + + +
- electron
- +
+ hole
+ + - -
- - - ++ + +
- - - + + + - -
+ + + - - -
+ + -
- - - + + +
+ + + - - -
- - - + + +
+ + + - - - EC
p-type material n-type material EC
EF EF
EC EC EV
EF
EV
EF
EV EV
Figure 15.5. When the p-type and n-type materials come
into contact, holes from the p side diffuse over to the n side,
and electrons from the n side diffuse over to the p side. As
Figure 15.4. Depiction of two semiconductor they do, they leave the host ions behind, which behave as
materials and their energy band diagrams, one of stationary space charge. Further, the Fermi energy level
which is p-type material and the other n-type ma- must be constant across the interface at equilibrium, hence
terial, suspended in vacuum before coming into the energy bands distort and bend as the system changes
contact. to the equilibrium condition.
636 Basics of Semiconductor Detector Devices Chap. 15

xp 0 xn
-x x
(a) Emax

- - - + + +
+ -
- - - + + +
(b) + -
- - - + + +
+ -
space-charge electron concentrations
region are equal above EC extending
from the p-type side.

EC
EC
(c) EF EF
EV
EV

hole concentrations are equal


below EV extending from the n-type side.

Figure 15.6. At equilibrium, the free carriers are swept from the
space-charge or depletion region, leaving behind a polarized zone that
produces an internal electric field. Hence diffusion of charges in one
direction is balanced by electric field drift in the other. Depicted in
the diagram are (a) the electric field, (b) the space-charge region,
and (c) the energy band diagram.

Width of the Space-Charge Region


To determine the width of the space-charge region, begin with Poisson’s equation and a few simplifying
assumptions. The general Poisson equation is
∇•D = ∇•[0 κE] = ∇•[0 κ∇V (r)] = ρc (r), (15.45)
D is the electrical displacement, 0 is the permittivity of free space, κ is the dielectric constant, E is the
electric field, V is the electric potential, and ρc is the volumetric charge density. For the one-dimensional
case with a constant permittivity, Eq. (15.45) reduces to
∂ 2 ψ(x) ρ(x) qe
2
=− = (NA− − ND
+
− p + n) (15.46)
∂x 0 κ s
where qe is the unit electron charge, ψ(x) is the scalar voltage component in the x direction (the y and z
voltage components are zero in the present example). Here n, p, ND +
, and NA− are the concentrations of the
Sec. 15.3. Basic Semiconductor Detector Configurations 637

free electrons, free holes, ionized donors, and ionized acceptors, respectively. Also the relation s = 0 κ has
been used. To simplify the problem further, the following approximations are made.
1. Assume that the junction is abrupt at the interface between the p-type side and the n-type side and
that all dopants in the materials are uniformly distributed.
+
2. Assume ND +
n, p, or NA for the n-type side and that ND  ND at 300 K.
3. Assume NA− n, p, or ND for the p-type side and that NA−  NA at 300 K.
Equation (15.46) then reduces to the following:
∂ 2 ψ(x) −qe ND
+
∂ 2 ψ(x) qe NA−
 , 0 ≤ x ≤ xn , and  , xp ≤ x ≤ 0, (15.47)
∂x2 s ∂x2 s
and outside the space-charge region ∂ 2 ψ(x)/∂x2 = 0, x ∈/ (xp , xn ).
The electric field on the n-type side of the junction is found by integration of Eq. (15.47) as

∂ψ(x) qe N D qe N D
− = E(x) = dx = x + C1 , 0 ≤ x ≤ xn , (15.48)
∂x s s
and the electric field on the p-type side is

∂ψ(x) qe N A qe N A
− = E(x) = − dx = − x + C2 , xp ≤ x ≤ 0. (15.49)
∂x s s
With the boundary conditions E(xp ) = E(xn ) = 0 the arbitrary constants C1 and C2 can be evaluated and
the electric field is found to be

⎪ qe N D

⎨  (x − xn ), 0 ≤ x ≤ xn
s
E(x) = . (15.50)

⎪ q N
⎩ − e A (x − xp ), xp ≤ x ≤ 0
s
Notice that the slope of the electric field magnitude is a linear function of the doping concentrations, ND
and NA . The electric field must also be continuous across the junction, hence at x = 0 one has
qe N D qe N A
− xn = xp so that ND xn = −NA xp . (15.51)
s s
These are important relations because they show that the relative width of the space charge region increases
as the doping concentration decreases. For instance, if ND is 10 times greater than NA , then for any given
applied voltage, xp must be 10 times greater than xn . Notice also that the largest magnitude of the electric
field must be at x = 0 (the pn junction interface), i.e.,
qe N D qe N A
Emax = − xn = xp . (15.52)
s s
The change in voltage across the space-charge region can be found by integration of electric field,
 xn  0  xn
qe NA qe ND
ΔV = − E(x) dx = (x − xp ) dx − (x − xn ) dx
xp xp s 0 s
qe : ;
= NA x2p + ND x2n . (15.53)
2s
638 Basics of Semiconductor Detector Devices Chap. 15

Hence, there is an electric field and a built-in voltage


space charge region potential Vbi at the pn junction without the need of any
- - - + + + externally applied voltage. Some semiconductor detec-
- - - + + + tors operate well on this built-in potential alone. The
built-in potential can be rewritten as
- - - + + +
- - - + + + qe : ;
Vbi = NA x2p + ND x2n
- - - + + + 2s
Emax Emax W
=− (xn − xp ) = − , (15.54)
junction

2 2
p-type n-type
where W = xn − xp is the total space-charge region
EC width as shown in Fig. 15.7. Typically, pn junction diode
qVbi detectors have a voltage applied in the reverse direction
to increase the width of the space-charge or active region.
EC With the second result of Eq. (15.51), Eq. (15.53)
EF EF can be rewritten as
p n
EV
 2 2 
qe ND xn 2
Vbi = + ND xn ,
EV 2s NA
xp 0 xn which, upon solving for xn , gives
Figure 15.7. At equilibrium in a pn junction, the free "  #1/2
charge carriers are swept from the space-charge or deple- 2s Vbi NA
xn = . (15.55)
tion region, leaving behind a polarized zone that produces qe ND (ND + NA )
an internal electric field. Diffusion of charges in one di-
rection is balanced by electric field drift in the other. At In the same way, Eq. (15.53) can be rewritten as
equilibrium, the Fermi level is constant across the junction.
At the pn junction, the energy bands bend and produce the * +
built-in potential Vbi . qe 2
NA2 x2p
Vbi = NA xp + ,
2s ND

whose solution for xp is


"  #1/2
2s Vbi ND
xp = − . (15.56)
qe NA (ND + NA )
Equation (15.55) and Eq. (15.56) can be combined to yield the active region width W , without a bias, as
" #1/2 "
  #1/2
2s Vbi
NA 2s Vbi ND
W = xn − xp = + ,
qe
ND (ND + NA ) qe NA (ND + NA )
" #1/2 $  / "  #1/2
2s Vbi NA ND 2s Vbi NA + ND
= + = . (15.57)
qe (ND + NA ) ND NA qe NA ND

When an external bias is applied, the active region width is


"  #1/2
2s (Vbi − V ) NA + ND
W = . (15.58)
qe NA ND
Sec. 15.3. Basic Semiconductor Detector Configurations 639

In the case that one side of the junction is doped much higher than the other side, by at least an order of
magnitude, Eq. (15.58) can be approximated by
" #1/2
2s (Vbi − V )
W  , (15.59)
qe Nb

where Nb is the doping concentration of the lighter doped side, commonly named the one-sided abrupt
junction approximation.
One can also calculate Vbi as a function of the extrinsic and intrinsic Fermi energies. From Fig. 15.7, it
is seen that qe Vbi equals the energy difference in the conduction band levels on the p-type side and on the
n-type side. Thus, Vbi can be calculated as
 
qe Vbi = (Ei − EF p ) p−type + (EF n − Ei ) n−type ,
     
pp nn nn pn
= kT ln + kT ln = kT ln .
ni ni ni 2

At room temperature pp  NA and nn  ND so that


 
kT ND NA
Vbi  ln . (15.60)
qe ni 2

Example 15.1: Consider a Si diode structure with a p-type dopant of concentration NA = 1017 cm−3
diffused into the surface of lightly doped n-type material that has a background concentration of ND = 1014
cm−3 . What is the built-in potential and total active region width at room temperature (300 K)?

Solution:

For Si s = 11.9o , and ni (300K) = 1.45 × 1010 cm−3 . Substitution into Eq. (15.60) gives
  : ; *: ;: ;+
kT ND NA 1.38 × 10−23 J/K (300 K) 1014 cm−3 1017 cm−3
Vbi = ln = ln : ;2 = 0.636 volts.
qe ni 2 1.6 × 10−19 C 1.45 × 1010 cm−3

From Eq. (15.58) the active region (or depletion region) width is
$   /1/2
2s (Vbi − V ) NA + ND
W = ,
qe NA ND

$   /1/2
(2)(11.9)(8.854×10−14 F/cm)(0.636 V−0 V) 1017 cm−3 + 1014 cm−3
= = 2.895 × 10−4 cm.
1.6×10−19 C (1014 cm−3 ) (1017 cm−3 )

Because the n-type side has a significantly lower doping concentration than the p-type side, one can also
use the approximation of Eq. (15.59) with Nb = ND to give
" #1/2 " #1/2
2s (Vbi − V ) (2)(11.9)(8.854 × 10−14 F/cm)(0.636 V − 0 V)
W  = = 2.894 × 10−4 cm.
qe Nb (1.6 × 10−19 C)(1014 cm−3 )

This result is essentially the same as the first solution.


640 Basics of Semiconductor Detector Devices Chap. 15

At room temperature, the material resistivity ρs can be expressed as ρs = 1/(qe μs Ns ), where Ns and
μs are the background dopant concentration and mobility for the lighter doped side of the junction, and
Eq. (15.59) can be rewritten as
W  {2s μs ρs (Vbi − V )}1/2 . (15.61)
The magnitude of the electric field across the device is
qe N s
|E(x)|  (W − x), 0 ≤ x ≤ W. (15.62)
s
Device Capacitance
The capacitance of a parallel contact pn junction detector is given by
s A
Cdet = , (15.63)
W
where A is the device active contact area. Substitution of Eq. (15.61) into Eq. (15.63) yields
1/2
s
Cdet  A . (15.64)
2μs ρs (Vbi − V )

Detector capacitance affects the input voltage pulse height, with a large capacitance diminishing the input
voltage from the detector that is measured by the amplification circuit such that
Q
Vin  , (15.65)
Ctot
where Ctot is the total capacitance (detector and coupling) and Q is the total charge collected from the
radiation detector after a radiation event. Hence, it is important to reduce detector capacitance and coupling
capacitance between the detector and the shaping electronics. From Eq. (15.64), it is seen that increasing the
reverse bias voltage decreases the detector capacitance, but at the expense of increasing the leakage current.
Fermi Level and Current at Equilibrium
The general equations describing current density for electrons and holes are given by Eqs. (15.29) and (15.30).
The total conduction current density is Jc = Jp + Jn . Under a condition of no applied external voltage and
equilibrium conditions, these currents must all vanish. Thus, in one dimension,

dp(x)
Jp (x) = qe μp p(x) E(x) − qe Dp = 0, (15.66)
dx
in which μp is the hole mobility, p is the hole concentration, and

dn(x)
Jn (x) = qe μn n(x) E(x) + qe Dn = 0. (15.67)
dx
where μn is the electron mobility, n is the hole concentration. There is a relative change in the intrinsic
Fermi level Ei (x) location, with respect to the band edges, across a pn junction. From the definitions of
qe V (x) = E(x) and Dn given by Eq. (15.31), Eqs. (15.66) and (15.67) can be written as

dEi (x) dp(x)


Jp (x) = μp p(x) − kT μp = 0, (15.68)
dx dx
Sec. 15.3. Basic Semiconductor Detector Configurations 641

and
dEi (x) dn(x)
Jn (x) = μn n(x) + kT μn = 0. (15.69)
dx dx
Eq. (12.130) can be divided by Eq. (12.128) to yield

EV − EF (x)
NV exp
p(x) kT Ei (x) − EF (x)
= = exp , (15.70)
ni EV − Ei (x) kT
NV exp
kT
which is an expression for p(x). The resulting derivative for dp/dx is then found to be

dp(x) ni (Ei (x) − EF (x)) dEi (x) dEF (x)


= exp − ,
dx kT kT dx dx
 
p(x) dEi dEF
= − . (15.71)
kT dx dx
Substitution of Eq. (15.71) into Eq. (15.68) gives
 
dEi (x) p(x) dEi dEF dEF
Jp (x) = μp p(x) − kT μp − = μp p(x) = 0. (15.72)
dx kT dx dx dx
A similar result can be derived for the n-type side, namely
dEF
Jn (x) = μn n(x) = 0. (15.73)
dx
so that the total current density is
dEF dEF
J(x) = Jp (x) + Jn (x) = μp p(x) + μn n(x) = 0. (15.74)
dx dx
Recall that the Fermi level at equilibrium is continuous across a boundary. The interpretation of Eq. (15.74)
is that the Fermi level at equilibrium is constant on the p and n sides of the junction, and must also be
constant across the junction, as shown in Fig. 15.8(e). Hence, at equilibrium, the net current must be zero.
Current Under Forward Bias
The current density of a pn junction diode is described by [Sze 1981]
" #
qe V
J = Js exp −1 , (15.75)
n̆kT
where n̆ is an ideality factor to correct for non-ideal behavior, and saturation current density Js is
qe Dp pno qe Dn npo
Js = + , (15.76)
Lp Ln
Dp is the diffusion coefficient for holes, Dn is the diffusion coefficient for electrons, pno is the minority hole
concentration in the n-type material, npo is the minority hole concentration in the p-type material, and the
diffusion lengths Lp and Ln are defined as

Lp,n = Dp,n τp,n . (15.77)
642 Basics of Semiconductor Detector Devices Chap. 15

space-charge
region
- - - - + +
+ + + -
- - - - +
(a) + + +
- - - - + +
+ + + -

NA - ND

0
xn
(b)
xp
r(x)

xp ++++++
(c) -0
- xn
-
-
-
-
xp 0 xn

(d) Emax

E electron concentrations
are equal above E extending
from the p-type side.

EC
(e) EF
EV

hole concentrations are equal


below EV extending from the n-type side.

Figure 15.8. The depleted region extends furthest into the junction region
of lowest doping. For the case in which the p-type region is of higher doping
levels than the n-type region, shown are (a) the device space-charge region,
(b) the dopant density, (c) the space-charge density (d) the electric field,
and (e) the energy band diagram.
Sec. 15.3. Basic Semiconductor Detector Configurations 643

Diffusion current -
not drift!
EC
Efn EC
p-type side n-type side
EF
+
EF
EV Efp _
EV

Figure 15.9. Diffusion current dominates in forward bias and, because of the
non-linear distribution of free carriers in the conduction and valence bands,
the observed current increases exponentially with increasing forward bias.

EC minority carrier injection


thermal charge carrier generation
tunneling
EF n >> p on n-type side
Efp
EV
n-type side
_
p-type side EC
+
Efn
EF
p >> n on p-type side
EV

Figure 15.10. In reverse bias, the density of available carriers, dominated by the
minority carrier concentration, determines the leakage current. At higher voltages,
bulk generation and tunneling may increase the observed leakage currents.

Here τp,n is the corresponding charge carrier lifetime. With a forward bias (see Fig. 15.9), the electron
distribution on the n-type side is raised in energy above the barrier on the p-type side, thereby allowing
diffusion of charge carriers to flow into the p-type side. According to the integrand of Eq. (12.120), the
electron distribution in the conduction band as a function of energy is non-linear, and the amount of current
increases exponentially as more forward voltage is applied. From the integrand of Eq. (12.123), the same
can be shown for holes diffusing from the p-type side over into the n-type side.
Also depicted in Fig. 15.9 are the quasi-Fermi levels Ef n for electrons and Ef p for holes.3 A quasi-Fermi
level describes the population of electrons and holes separately in the conduction band and valence band
when no longer in equilibrium, such as the case with applied voltage (forward or reverse) or other cases of
charge injection, such as photoexcitation.
Leakage Current Under Reverse Bias
There are three main sources of leakage current, as depicted in Fig. 15.10. Although the majority carriers
on the p-type side are holes, according to Eq. (12.131) a small concentration of electrons is still present.
These minority charge carriers (electrons) can diffuse into the depletion region, where they are swept across
by the electric field and contribute to the leakage current. A similar case is true for holes diffusing from the
n-type side into the depletion region. Leakage current can also occur from thermal generation of electrons
directly across the band gap into the conduction band, producing electron and hole free carriers. Thermal
generation of such charge carriers can be suppressed by cooling the detector while it is operating. Under high

3A quasi-Fermi level is also called an ‘imref’, the word ‘fermi’ spelled backwards [Hannay 1959].
644 Basics of Semiconductor Detector Devices Chap. 15

voltage bias conditions, charge carriers can also tunnel directly across the band gap, again contributing to
the leakage current. Variations about the leakage current can be a significant source of electronic noise (shot
noise), which broadens the overall energy resolution of the detector. Basically, pn junctions are employed to
minimize leakage currents in semiconductor detectors.

Example 15.2: Given a silicon pn junction with NA = 1015 cm−3 and ND = 1013 cm−3 , what is the
minority carrier saturation leakage current density under reverse bias at 300 K? The electrons and hole
mobilities are and 1320 cm2 V−1 s−1 and 470 cm2 V−1 s−1 , respectively (see Fig. 16.3), with τn,p = 10−3 s.

Solution:
From Eq. (15.31)
μkT
D=
qe
we have
(470 cm2 V−1 s−1 )(1.38 × 10−23 J K−1 )(300 K)
Dp = = 12.16 cm2 s−1 .
1.6 × 10−19 C
and
(1320 cm2 V−1 s−1 )(1.38 × 10−23 J K−1 )(300 K)
Dn = = 34.16 cm2 s−1 .
1.6 × 10−19 C
Because np = n2i , one has
  *<  +
Dp pn0 Dn np0 Dp Dn
Js = qe + = qe n2i + ,
Lp Ln n2 τp p 2 τn

which gives
*< < +
−19 10 −3 2 12.16 cm2 s−1 34.16 cm2 s−1
Js = (1.6 × 10 C)(1.5 × 10 cm ) + ,
(10 cm−3 )2 (10−3 s)
13 (10 cm−3 )2 (10−3 s)
15

= 4.04 × 10−14 amperes

Use of Reverse Bias


The active radiation-sensitive volume of the pn-junction detector is defined by the space-charge region (or
depletion region), and the undepleted regions act as series resistances. Detectors based on pn junction diodes
are typically operated under reverse bias, which is regarded as a negative voltage, but is actually a positive
voltage applied to the n-type material with respect to the p-type material. Shown in Fig. 15.10 is the band
diagram of a reverse biased pn junction. The large energy band barriers prevent electrons on the n-type side
from diffusing over to the p-type side and prevent holes on the p-type side from diffusing into the n-type
side. There remains the possibility of electrons on the p-type side diffusing to the n-type side, and holes on
the n-type side diffusing into the p-type side, both of which produce current. However, from Eq. (12.131),
the density of minority carrier holes and minority carrier electrons is small (depicted in Fig. 15.10), and
consequently the leakage current is small. As a result, the pn junction suppresses leakage current that would
be present if the semiconductor were operated as a resistor. This necessary condition reduces the electron
current such that minute charge packets excited in the depletion region by radiation interactions can be
measured.
Sec. 15.3. Basic Semiconductor Detector Configurations 645

E E E
xp 0 xi xn xp xp 0 xn xp 0 xn xn

(a)

Emax Emax Emax

p-type intrinsic n-type p-type p-type n-type p-type n-type n-type


(b) region region region region region region region region region

EC EC EC
EC EC EC
(c) EF EF
EF
EF
EF
EF
EV EV EV
EV EV EV
pin ppn pnn
Figure 15.11. Electric field (a), material regiobs (b), and band diagrams (c) of pin, pπn and pνn devices. Note that
the electric field across the intrinsic region of the pin diode is constant, but the lightly doped pπn and pνn have a
definite slopes to their electric fields.

15.3.2 pin Junction Devices


Reverse biased diode detectors need a large depletion region to maximize radiation absorption. As found
in Eq. (15.58), the depletion region width is proportional to the square root of the applied reverse voltage.
This relationship indicates large voltages are required to produce large depletion regions in a common pn
junction diode. The usual remedy to avoid high voltages is to construct a pin diode that has an intrinsic,
or high purity region, between the p-type and n-type contacts. The p and n type contacts can be used as
either blocking barriers or electrical ohmic contacts to the material. The application of p-type contacts to
p-type material, or n-type contacts to n-type material, generally produce non-rectifying electrical contacts
that follow Ohm’s law.
A pin device may have a truly intrinsic region between the p and n type contacts, in which the electron
and hole populations are identical, or the high purity region may be a lightly doped material. Lightly doped
p-type material is commonly denoted π-type, and lightly doped n-type material is commonly denoted ν-
type. Analysis of the diode construction should take into account the “punch-through” voltage, in which the
depletion region extends completely across the high purity region, whether the material is i, ν, or π type.
Semiconductor pin diode radiation detectors are commonly operated at biases above the punch-through
voltage.
Intrinsic material either has dopant concentrations below the intrinsic concentration or has compensation
dopants that cause the residual free carrier concentration to be below the intrinsic concentration. In either
case, the residual space charge is practically zero (ρc  0), and from Eq. (15.46) the resulting electric
field is constant across the pin diode under reverse bias. Many detectors are fashioned from high-purity
semiconductor materials, yet such detectors may not behave intrinsically, because of a small concentration
of residual dopants that is still above the intrinsic concentration. As a result, ρc is non-zero, even if very
small, and the depletion region width is determined by Vbi and the applied voltage. If the lightly doped π
or ν regions are relatively thin, the detector might become “fully depleted” without an applied voltage, as
depicted in Fig. 15.11. However, complete depletion is usually not the case, and a reverse bias must then be
646 Basics of Semiconductor Detector Devices Chap. 15

applied to extend the depletion region and the electric field across the device, as determined from Eq. (15.58)
and Eq. (15.59), respectively.

Example 15.3: Given a silicon pνn diode with NA = 1015 cm−3 , Nd = 1013 cm−3 , and ND = 1015 cm−3 ,
what is the depletion width for a 450 micron thick ν region with a bias of 200 volts reverse bias? With Nd
reduced to 1012 cm−3 , what is the depletion width at 100 volts reverse bias?

Solution:
The one-sided abrupt junction approximation is used in the first case.
 <
2κo V (2)(11.9)(8.854 × 10−14 F cm−1 )(200 volts)
W  = = 162.3 microns.
qe Nd (1.6 × 10−19 C)(1013 cm−3 )

The ν region dopant concentration is now reduced to 1012 cm−3 , yielding,


 <
2κo V (2)(11.9)(8.854 × 10−14 F cm−1 )(200 volts)
W  = = 513.2 microns,
qe Nd (1.6 × 10−19 C)(1012 cm−3 )

which is wider than the ν region. Hence, in the second case the diode is fully depleted with W = 450
microns.

15.3.3 Metal-Semiconductor Contacts


Consider a situation in which a metal block and a semiconductor block are both suspended in free space,
and that somehow they are spontaneously fused together. What then would happen? Entire books have
been published on the physics of metal-semiconductor contacts. Such depth of coverage is not possible here;
however, those major concepts, important to the design and fabrication of semiconductor detectors, are
briefly presented.
Schottky Devices
Earlier it was shown that the Fermi energy level must be constant at equilibrium. Further, if the derivative of
the Fermi level with respect to position were to change, it would imply the presence of current flow. However,
it can be readily assumed that a free floating semiconductor substance onto which a metal is attached does
not have current flowing through the structure. Hence, the Fermi level must remain constant. As a metal
and semiconductor are brought together, the energy bands must deform to (1) ensure that the vacuum level
is continuous and (2) ensure that the Fermi level is constant.
The application of a metal to a semiconductor surface acts to bend the semiconductor bands to form an
energy barrier qe φbn , much like the pn junction diode, as shown in Fig. 15.12. The Fermi energies, defined
by the metal and semiconductor work functions (φm and φs ) must align when the two materials are brought
into contact.
Shown in Fig. 15.12(a) are depictions of the energy bands for a metal and a semiconductor. The vacuum
levels of both materials are continuous. The work functions of both materials are defined as the difference
between the vacuum level and Fermi levels. Given a temperature and pressure, the work function of the
metal, qe φm , may be regarded as a constant. However, the Fermi level of a semiconductor, qe φs , is a
function of doping concentration, and, hence, is not considered a constant reference point. Instead, the
electron affinity, qe χs , defined as the difference between the vacuum level and the conduction band edge, is
generally used as a constant of reference. As the junction reaches equilibrium, the Fermi level on the metal
Sec. 15.3. Basic Semiconductor Detector Configurations 647

metal semiconductor metal semiconductor

vacuum level
qcs vacuum level
qfs qfm
qfm EC qfbi qfs qcs
EFs qfbn EC
EFm EFm
EV EFs
EV

(a) (b)

Figure 15.12. The band configuration depicted for a metal and semiconductor (a) before
and (b) after contact, according to the Schottky-Mott model.

and semiconductor sides must align. As a result of the junction formation, a built-in potential qe φbi forms
and a potential barrier qe φbn forms. The final barrier height is given by

qe φbn = qe (φm − χs ), (15.78)

and the built in potential is


qe φbi = qe (φm − φs ). (15.79)
This result is called the simple Schottky model. Under a reverse bias, this energy barrier serves to reduce
leakage current. Typically the barrier height is lower than that for pn or pin junction diodes, hence detectors
based on the Schottky barrier diode typically have higher leakage currents than pn or pin diodes.
Schottky Effect
Consider a single point charge in vacuum, an electron for instance, placed near the surface of a conductor
at distance x, as shown in Fig. 15.13. The point charge repels similar charges in the metal, leaving a net
positive charge on the surface, thereby giving the appearance of a positive charge of equal magnitude in the
metal at the distance −x from the metal surface. The forces exerted upon the point and image charges are
equal and opposite, namely  
qe2  −qe2 
F =  = . (15.80)
4πs (2x)2 point 4πs (2x)2 image
The potential due to the image force is found as
 x
−qe2
V1 (x) = F dx = , (15.81)
∞ 16πs x

and the electric field potential is V2 (x) = −qe xE. Therefore, the total energy is

−qe2
Vtot = V1 + V2 = − qe xE. (15.82)
16πs x
The situation is depicted in Fig. 15.14, in which the total potential of the image charge has a maximum
value at qe Δφ located at xm from the metal/vacuum interface.
648 Basics of Semiconductor Detector Devices Chap. 15

metal vacuum
metal E vacuum
xm x
2
qDf -q
+ - 16peox

qfE -qxE

Ef
-x x
Figure 15.13. A single point charge in vac- Figure 15.14. Schottky barrier lowering re-
uum, such as an electron, near a conductive sults from the combined effects of the image
surface effectively produces an image charge of and electric field potentials.
opposite magnitude to appear in the conductor.

The Schottky barrier effect thus lowers the Schottky barrier by an amount qe Δφ. This barrier lowering
occurs at xm , where the electric field has a maximum Em . The distance xm can be found by setting the
derivative of Eq. (15.82) to zero, i.e.,
 
d −qe2  qe2
− qe xEm  = − qe Em = 0. (15.83)
dx 16πs x xm 16πs x2m

Solution of Eq. (15.83) for xm gives 


qe
xm = , (15.84)
16πs Em
from which the maximum field strength is
qe
Em = . (15.85)
16πs x2m
The change in the Schottky barrier height is
 
qe qe qe Em
Δφbi = xm Em + = 2xm Em = 2Em = , (15.86)
16πs xm 16πs Em 4πs
which is also the potential of Schottky barrier lowering. What this result means is that the actual Schottky
barrier for the diode is lower than expected from the simple Schottky model. The end result is a barrier
height of
qe φbn = qe (φm − χs − Δφbi ). (15.87)
Bardeen Model: Surface State Effects
It should be noted that measured Schottky barrier heights typically do not match the theoretical values,
even after considering the Schottky lowering effect. In fact, quite often the actual barrier height φbn is only
modestly affected by φm , or in some cases the final barrier height φbn appears to be completely independent
of the metal.
Sec. 15.3. Basic Semiconductor Detector Configurations 649

Because the surfaces of semiconductors have defects, vacuum level


interface states, and possible contaminants, the actual
barrier height depends not only upon the choice of metal qcs qfs
but also on how the surface is prepared. These surface qfm surface bulk
states can effectively “pin” the detector barrier height, EC
thereby predetermining the actual value of qe φbn before

EFs
the metal is applied. Bardeen offered an explanation to
EFm
the difference by taking into account the effect of inter- EFs
face states on the Schottky barrier. qfo
Assume that there is an unspecified density Ds (in EV
units of eV−1 cm−2 ) of unbonded states upon the surface
of a semiconductor material. These unbonded states can
arise from a combination of open bonds from the semi-
conductor host atoms, referred to as Tamm-Shockley Figure 15.15. Band conditions for an n-type semicon-
states, and also from contaminate atoms attached to the ductor with a high density of surface states, showing the
neutral level qe φo . States below qe φo are donors and states
surface. The surface states are classified donor states if above qe φo are acceptors.
they are neutral when occupied, and these states are
classified as acceptor states if they are neutral when empty. Fast surface states are close to the bulk material
and reach equilibrium quickly with a rapid change in potential. Slow surface states are further from the bulk
material and take a relatively longer time to reach equilibrium with a potential change.
Now assume that there is a thin interfacial insulator region δ between the metal and the semiconduc-
tor that is capable of supporting a potential. Also assume that the surface states are a property of the
semiconductor alone and are independent of the metal. The states must be either filled or empty, and the
filled surface states produce image charges of the opposite polarity in the semiconductor. In other words,
for n-type material, a space-charge (depletion) region forms from the repulsion of electrons at the surface,
and the bands bend to accommodate the potential formed at the surface. Overall, a specific density of these
states is filled up to a neutral level qe φo = Eo , as depicted in Fig. 15.15. The states below the neutral level
are filled donor states and hence are neutral, and the states above the neutral level are empty acceptors and
are also neutral. If the Fermi level is raised to Ef , then some of the surface acceptor states become filled
and produce a net negative surface charge.
The surface charge Qss density, in units of C cm−2 , is
Qss = −qe Ds [Eg − qe Δφbi − qe φbn − qe φ0 ] , (15.88)
in which φbn is the energy barrier height at the metal-semiconductor interface. According to Gauss’ law, the
semiconductor and metal cannot support an electric field, hence
i Ei = Qss = −Qm , (15.89)
where i is the permittivity of the thin interface insulator, and Qm is the mirror charge formed on the metal.
The voltage across the thin insulator is
δQss
Vi = δEi = . (15.90)
i
As depicted in Fig. 15.16, the metal work function is,
qe φm = qe Vi + qe χs + qe φbo , (15.91)
and therefore the barrier height is
δQss
qe φbo = qe φm − qe χs − qe . (15.92)
i
650 Basics of Semiconductor Detector Devices Chap. 15

Substitution for Qss from Eq. (15.88) gives


qVi qe δDs [Eg − qe Δφbi − qe φbn − qe φ0 ]
qe φbo = qe φm − qe χs + .
qcs i
(15.93)
qDfbi
qfm qfbi Define ζ ≡ i /(i + qe δi Ds ), and substitute it into Eq. (15.93) to
qfbo EC obtain
qfbn  
Eg
EF φbo = qe φbn + Δφbi = ζ(φm − χs ) + (1 − ζ) − φo . (15.94)
qfo qe
As the width δ of the thin interface insulator decreases to zero,
d EV ζ → 1 and Eq. (15.94) reduces to
φbn = φm − χs − Δφbi , (15.95)
Figure 15.16. Band conditions for an n-type which is the expected result of Eq. (15.87) found earlier. If the
pinned Schottky barrier, showing the neutral surface state density becomes large, then ζ → 0 and Eq. (15.94)
level qe φo , below which states are filled and above becomes
which states are empty. The shaded regions in- Eg
dicate energy bands with allowed states. φbn = − φo − Δφbi . (15.96)
qe
The barrier height is no longer a function of the Fermi energy,
but is instead a function of the neutral surface state energy. Note
qfbi
that the neutral level may not be at the same energy as the bulk
qfbn EC Fermi energy. The Fermi level in the semiconductor bulk must
remain constant under equilibrium conditions, hence, if Eo is
EF
below EF s , the bands must bend up (as shown in Fig. 15.17)
until the Fermi level is aligned with Eo . If the neutral level Eo
is above EF s , then the energy bands must move downwards. In
EV Fig. 15.18 the interface states and band conditions are shown for
n-type and p-type Schottky barriers.

Depletion Region
Figure 15.17. Band conditions for an n-type The electric field and the depletion region width can be calcu-
pinned Schottky barrier, showing the Fermi en- lated from the one-dimensional Poisson’s equation
ergy pinned at the neutral level qe φo .
d2 ψ dE(x) ρc (x)
2
=− =− , (15.97)
dx dx s
where ψ(x) is the voltage or potential in the device. Thus, Eq. (15.97) for n-type material becomes
+
d2 ψ(x) dE(x) qe N D
= − = − , (15.98)
dx2 dx s
and for p-type material
d2 ψ(x) dE(x) qe NA−
2
=− = . (15.99)
dx dx s
At room temperature, it is reasonable to assume that the shallow dopants are fully ionized, i.e., NA−  NA
and ND+
 ND . For an n-type Schottky contact, the electric field is
 
dE(x) qe ND qe N D
E(x) = dx = dx = x + C. (15.100)
dx s s
Sec. 15.3. Basic Semiconductor Detector Configurations 651

vacuum level
vacuum level qcs
qfs
qfm qfm
qfs qcs EC
qVbi EC
qfbn
EFm EFm EFs
EFs qfbp
qVbi EV
metal metal
EV
semiconductor semiconductor
n-type Schottky barrier p-type Schottky barrier

Figure 15.18. Interface states and band conditions for n-type and p-type “pinned” Schottky
barriers.

With the boundary condition E(xn ) = 0, the integration constant C in the above result is found to be
C = −(qe ND xn )/s , and the electric field is thus

qe N D
E(x) = (x − xn ). (15.101)
s

The built-in potential is then evaluated as


 xn  xn
qe ND qe ND x2n
Vbi = − E(x)dx = − (x − xn )dx = . (15.102)
0 0 s 2s

Rearrangement of terms and inclusion of a reverse bias voltage yield the width of the depletion region as
" #1/2
2s (Vbi − V )
W = , (15.103)
qe ND

a result similar to that for a one-sided abrupt pn junction.


For p-type Schottky junctions, it can be shown in a similar fashion

qe N A
E(x) = (xp − x), (15.104)
s

and
" #1/2
2s (Vbi − V )
W = . (15.105)
qe NA
Just as Eq. (15.59) can be rewritten as Eq. (15.61), Eqs. (15.103) and (15.105) can be rewritten as
1/2
W  {2s μs ρs (Vbi − V )} . (15.106)

The value of Vbi for common Schottky diodes is 0.3 volts. Note that Schottky contacts can be formed
on n-type or p-type semiconductors, as depicted in Fig. 15.19. Besides being simple to construct, Schottky
barrier detectors have a thin entrance region at the contact, unlike most pn and pin diodes, and energy
attenuation in this “dead region” is kept to a minimum. As a result, Schottky barrier detectors (sometimes
called “surface barrier detectors”) are useful as charged-particle spectrometers.
652 Basics of Semiconductor Detector Devices Chap. 15

vacuum level
vacuum level qcs
qfm
Schottky
qfs qcs EC
contact tunnel
contact
qVbi EC qfm qfs
qfbn e-
EFs EFm
EFm EFs qfbp
qVbi EV e-
tunnel
Schottky contact
EV
contact
n-type Schottky barrier diode p-type Schottky barrier diode

Figure 15.19. Interface states alter the interface potentials and effectively “pin” the Schot-
tky barrier. Shown are n-type and p-type Schottky barriers, along with n-type and p-type
tunneling ohmic contacts.

Current Under Forward Bias


The current density of a Schottky barrier rectifying junction can be written as [Rhoderick and Williams
1988]  
qe V
J = Js exp −1 , (15.107)
kT
and
qe φbn
Js = A∗ T 2 exp − . (15.108)
kT
and A∗ is the effective Richardson constant. Under forward bias, the majority carrier concentration is
elevated in energy above the semiconductor barrier φbi , thereby allowing a non-linear supply of electrons to
diffuse across the junction.
In the case that the Schottky barrier height is affected by a bias voltage, an additional change must be
included
φbn = φm − χs − Δφbi + βV = φbn + βV, (15.109)
where the coefficient β is positive for forward bias [Rhoderick and Williams 1988]. Substituting φbn for φbn
into Eq. (15.107) yields  
−βqe V qe V
J = Js exp exp −1 , (15.110)
kT kT
The ideality factor is defined as
1
n̆ = , (15.111)
1−β
which, upon substitution into Eq. (15.110), yields
 
qe V −qe V
J = Js exp 1 − exp . (15.112)
n̆kT kT
For large values of V (> 3kT /qe ), Eq. (15.112) can be approximated by
qe V
J ≈ Js exp . (15.113)
n̆kT
Sec. 15.3. Basic Semiconductor Detector Configurations 653

Thermally excited carriers surmounting the barrier


Carriers tunneling through the barrier
EFm EFsp

_ EC +
EFsn EFs

EV
Carrier generation-recombination
Figure 15.20. Energy band diagram for an n-type Schottky contact under
reverse bias.

Reverse Leakage Current Under Reverse Bias


Sources of leakage current are shown in Fig. 15.20. Unlike the pn junction device, there is no supply of
“minority” carriers at the junction boundary. Instead, there is a reservoir of free electrons from the metal,
which must surmount the energy barrier before they can enter the semiconductor. Hence, the reverse bias for
a Schottky barrier is a function of the barrier height φbn . Under reverse bias, these charge carriers (electrons)
can be elevated by thermionic emission over barrier and contribute to the leakage current. A similar situation
occurs for holes with a p-type Schottky contact. Leakage current can also occur from thermal generation of
electrons directly across the band gap into the conduction band, producing electron and hole free carriers.
Similar to the pn junction device, thermal generation can be suppressed by cooling the device while under
operation. Finally, under high voltage bias conditions, charge carriers can tunnel quantum mechanically
directly through the energy barrier, thereby also contributing to the leakage current.
Junction Breakdown
In Sec. 14.2.3, the concept of diode breakdown was briefly discussed as an introduction to SPAD and SiPM
light detection devices. The phenomenon of breakdown can also be observed in semiconductor diodes such
as pn, pin, and Schottky devices. Breakdown can be recognized as a tremendous increase in leakage current
at bias voltages past a specific threshold. Two mechanisms can describe this junction breakdown, namely,
tunneling and avalanche breakdown.
Tunneling Breakdown Under high reverse bias conditions, it is possible to cause such band bending across
a pn junction that electrons can tunnel directly from the valence band into the conduction band. Such a
condition is shown in Fig. 15.10 as a potential source of leakage current. In some circumstances, pn junction
diodes are fabricated with relatively high dopant concentrations with the intentional purpose of causing this
kind of breakdown. Such devices are called Zener diodes,4 and are commonly used for overvoltage circuit
protection. Typically, electric fields exceeding 106 V cm−1 are needed to achieve the band bending required
for Zener breakdown in specially designed highly doped pn junctions [Grove 1967]. Radiation detectors
are usually fabricated from high purity materials, and Zener breakdown is usually not reached before other
breakdown mechanisms are reached. Other breakdown mechanisms are usually of more concern.
Avalanche Breakdown The topic of avalanche breakdown was discussed earlier in Sec. 14.2.3. Indeed,
some light detection devices were seen to rely upon this effect for gain. However, avalanche breakdown can
become a source of unwanted noise and can also cause irreparable damage to semiconductor detectors. The

4 Named after Clarence M. Zener who discovered the effect.


654 Basics of Semiconductor Detector Devices Chap. 15

breakdown occurs when electrons gain enough kinetic energy from an applied electric field such that some
of their energy can be transferred to the lattice and excite more electrons into the conduction band.
Consider a uniformly doped semiconductor upon which is formed an abrupt one-sided rectifying junction.
From Eqs. (15.50) and (15.52), the general expression for the applied voltage is
 W  W
qe Nb W x W
V = E(x)dx = − 1 dx = −Emax , (15.114)
0 0 κo W 2
where Nb is the doping concentration of the lower doped side and W is the depletion width. Suppose that
Emax is the critical field required for avalanche breakdown. Then the magnitude of the breakdown electric
field is
2VB 2(Vbi − Vrev )
|Ecrit | = = , (15.115)
W W
where VB is the breakdown voltage and Vrev is the applied reverse voltage. Substitution of the one-sided
depletion approximation into Eq. (15.115) yields

Ecrit
2
κo
VB = Vbi − Vrev = . (15.116)
2qe Nb
The breakdown voltage of Si, Ge, and
GaAs as a function of background doping con-
centration was studied by Sze and Gibbons
[1966a] and the experimental measurement re-
sults shown in Fig. 15.21. Sze and Gibbons
[1966a] offer the following empirical relation to
estimate the breakdown voltage
 3/2  −3/4
Eg Nb
VB  60 in volts,
1.1 1016
(15.117)
where Nb is the background impurity concentra-
tion and Eg is the band-gap energy in electron
volts. A comparison of Eq. (15.117) with the
measured data is also shown in Fig. 15.21. It
appears that Eq. (15.117) yields acceptable re-
Figure 15.21. Avalanche breakdown voltage as a function of doping sults for background doping concentrations be-
concentration for an abrupt one-sided pn junction diode. A compar- low 1017 cm−3 , but is less accurate at higher
ison is made between the data of Sze and Gibbons [1966a] and the
empirical formula of Eq. (15.116).
doping levels. It is shown in Fig. 15.21 and
also Eq. (15.117) that the breakdown voltage
increases with band-gap energy. Intuitively, this observation makes sense, because wider band-gap materials
require more energy, on average, to produce an electron-hole pair than do narrow band-gap materials.
Another breakdown mechanism is a lowering of the breakdown voltage from rounded junction interfaces.
When dopants are introduced into substrates, the contact pattern is often defined by photolithography
methods. Doped patterns of specific size and shape are defined by windows etched through diffusion masks,
commonly a layer of SiO2 or other high-temperature insulator. Dopants are introduced by various methods,
including diffusion and implantation (for details, see Sze [VLSI 1985 and others]). These dopants are heated
to high temperatures to drive them into the substrate, and in doing so, they diffuse from high to low
concentrations. Consequently, at the pattern edges, it is usually the case that the junction interface becomes
Sec. 15.3. Basic Semiconductor Detector Configurations 655

rounded in a semi-cylindrical volume, with radius rj , as the dopants diffuse laterally from the point of
introduction. At the pattern corners, the combined edges form a hemispherical interface. Recall from
Sec. 8.7 and Sec. 8.8 that the electric field is higher at the smaller terminal than the larger terminal for
cylindrical and hemispherical geometries. Hence, the electric field formed around the pattern edges is higher
than expected with a simple planar pn junction. The overall effect is to lower the breakdown voltage of
the pn junction [Armstrong 1957]. Reported results by Sze and Gibbons [1966b] on Si diodes with different
junction curvatures are shown in Fig. 15.22.
Ghandhi [1977] offers an empirical relation  

to determine the breakdown voltages VJB of


  
curved junctions in Si abrupt one-sided pn junc-

   !" #


  
tions. For cylindrical junctions

#& 
$
VJB
= 0.5(η 2 + 2η 6/7 ) ln(1 + 2η −8/7 ) − η 6/7 , 

VB
(15.118)
and for spherical junctions %

VJB
= η 2 + 2.14η 6/7 − (η 3 + 3η 13/7 )2/3 ,
VB
(15.119)
where VB is the breakdown voltage for the

dopant concentration and     

rj      


η= (15.120)
W Figure 15.22. Breakdown voltage versus impurity concentration
for one-sided abrupt junction Si diodes with different cylindrical and
where W is the depletion width of the material spherical curvatures. Data from Sze and Gibbons [1966b].
at VB and rj is the radius of curvature. The
results from Eqs. (15.118) and (15.119) are shown in Fig. 15.23.

Figure 15.23. Normalized junction breakdown (VJ B /VB ) as a func-


tion of η = rj /W for cylindrical and hemispherical junctions in Si.
After Ghandhi [1977].
656 Basics of Semiconductor Detector Devices Chap. 15

Example 15.4: An abrupt p-type junction is diffused into a silicon substrate having an n-type background
concentration of 1015 cm−3 . The edges are cylindrical with a radius of curvature equal to 1 micron. What
is the junction breakdown voltage?

Solution:
First find the breakdown voltage from Eq. (15.117).
 3/2  −3/4  3/2  15 −3/4
Eg NB 1.12 eV 10
VB  60 = 60 = 346.65V.
1.1 1016 1.1 1016
Next find the depletion width at VB .
 <
2κo VB 2(11.9)(8.854 × 10−14 F/cm)(346.65 V)
W = = = 0.00214 cm.
qe Nb (1.6 × 10−19 C)(1015 cm−3 )
Determine the value of η from Eq. (15.118),
VJ B
= 0.5(η 2 + 2η 6/7 ) ln(1 + 2η −8/7 ) − η 6/7
VB
 2  6/7    −8/7   6/7
1 μm 1 μm 1 μm 1 μm
= 0.5 +2 ln 1 + 2 − = 0.2369.
21.4 μm 21.4 μm 21.4 μm 21.4 μm

The junction breakdown voltage is thus determined to be VJ B = 0.2369(346.65 volts) = 82.12 volts.

Punch Through Breakdown Semiconductor radiation detectors are usually fabricated from relatively
pure materials with low background impurity concentrations. Consequently, it is possible to fully deplete
a pn, pνn, or pπn diode, a condition called
Ecrit punch through. As the voltage is increased, the
maximum electric field also increases at the pn
junction. At high enough voltages, the elec-
tric field reaches the critical field required for
avalanching and reach a condition named punch
through breakdown.
ED
Consider Fig. 15.24, in which an ideal elec-
tric field is depicted for an abrupt one-sided
x junction for a uniformly doped substrate. For
0 D W a relatively thick substrate, a depletion width
Figure 15.24. The breakdown electric field is a function of the W is reached at the required breakdown elec-
background doping and space charge. The integral of the electric tric field Ecrit , where W can be found with
field as a function of x yields the resulting breakdown voltage, which Eq. (15.115). The breakdown voltage VB is de-
is also a function of the substrate width.
scribed by Eq. (15.116) and can be estimated by
Eq. (15.117); hence Ecrit can be determined.
If instead the width of the substrate is less than W , labeled D in Fig. 15.24, the integral of the electric
field yields the applied voltage, depicted by the shaded area of Fig. 15.24,
 D
V = E(x)dx.
0
Sec. 15.3. Basic Semiconductor Detector Configurations 657

Recall that the solution for the electric field in 

a uniformly doped pn junction yields a simple


! "
linear equation, shown in Eq. (15.50) with slope
(qe Nb )/(κo ). Using simple geometric analysis 

   


with Fig. 15.24, the punch through breakdown  
voltage VBP is


(Ecrit +ED )D 2 D D 
VBP = VB = VB 2− .
2 Ecrit W W W  
(15.121)
Insertion of Eq. (15.59) and the relation Vbi −V = 

VB yields 

    
   

       

qe Nb qe Nb
VBP = VB D 2−D .        
2κo VB 2κo VB
(15.122) Figure 15.25. Breakdown voltage for Si pνn and pπn diodes
as a function of background doping concentration and substrate
Shown in Fig. 15.25 are the dependences of VBP thickness determined from Eq. (15.117) and Eq. (15.122).
on doping concentration for several values of D
for silicon diodes.

Example 15.5: Given a 100-micron thick silicon pνn diode with NA = 1015 cm−3 , Nd = 1014 cm−3 , and
ND = 1015 cm−3 , what is the punch through breakdown voltage?

Solution:
First find VB by estimating the value with Eq. (15.117) or reading from the graph in Fig. 15.21.
 3/2  −3/4  3/2  −3/4
Eg NB 1.12 eV 1014
VB  60 = 60 = 1949V.
1.1 1016 1.1 1016

At a voltage bias of 1949 volts, the expected depletion width is,


 <
2κo VB 2(11.9)(8.854 × 10−14 F/cm)(1949 V)
W = = = 0.016 cm.
qe Nb (1.6 × 10−19 C)(1014 cm−3 )

Consequently, at VB , the diode is fully depleted and punched through. The punch through breakdown
voltage is found with Eq. (15.121),

D D
VBP = VB 2− ,
W W
0.01 cm 0.01 cm
= (1949 V) 2− ,
0.016 cm 0.016 cm

= 1674.9 V.

The punch through breakdown voltage VBP is 85.94% of the breakdown voltage VB .
658 Basics of Semiconductor Detector Devices Chap. 15

15.3.4 The MOS Structure


Another common semiconductor device structure is the metal-oxide-semiconductor (MOS) capacitor. Radi-
ation detectors usually do not have these structures, but there are some special radiation detection devices
that operate with MOS capacitors. For that reason, this design and the operating physics are briefly dis-
cussed here. A MOS structure has three basic components, the semiconductor, the insulating oxide layer
and a metallic gate upon the oxide as shown in Fig. 15.26. The MOS field effect transistor, or MOS-FET,
also has an injecting source contact and a receiving drain contact.
An ideal MOS capacitor can be described as a structure in which both the metal work function φm and
the semiconductor work function φs are equal, i.e.,
Eg
qe φm − qe φs = qe φm − qe χs − − |qe ψB | = 0, for p-type, (15.123)
2
and
Eg
qe φm − qe φs = qe φm − qe χs − + |qe ψB | = 0, for n-type. (15.124)
2
The MOS band structures for p-type and n-type substrates are depicted in Fig. 15.27. Hence, at zero voltage,
the band structures have constant energy so they are flat. Further, the insulating oxide region of an ideal
MOS device has no space charge imperfections and so there is no trapped charge at the oxide-semiconductor
interface. Finally, the oxide acts as a perfect insulating barrier and no leakage current penetrates the oxide
during operation. These conditions define an ideal MOS capacitor.

metal oxide source gate oxide drain


d d
semiconductor p-type

ohmic contact n-type n-type

(a) (b)
Figure 15.26. Cross section depiction of the main structural components of a (a) MOS
capacitor and a (b) MOS field effect transistor.

The band structure of an ideal p-substrate MOS capacitor under bias is depicted in Fig. 15.28. Note that,
because the oxide is a “perfect” insulator, no current can flow across the barrier, hence the Fermi energy
level remains flat even under bias. If a net negative bias is applied to the gate metal, then the energy bands
bend upwards, as shown in Fig. 15.28(a), and a potential well forms at the interface. The concentration of
the majority carrier holes is
Ei − EFs
pp = ni exp , (15.125)
kT
and at the oxide-semiconductor interface Ei − EF becomes relatively large. Consequently, holes gather at
the interface, a condition termed accumulation. A similar case occurs on a n-type substrate under positive
bias in which the majority carriers are electrons which accumulate at the interface so that
EFs − Ei
nn = ni exp . (15.126)
kT
Likewise the application of a small positive bias on the gate of a p-type MOS capacitor causes the
energy bands to bend downwards, ultimately reducing the number of holes at the interface, thereby causing
Sec. 15.3. Basic Semiconductor Detector Configurations 659

vacuum level vacuum level

qfB qcs qfs Eg qfB qcs qfs Eg


2 2
qfm qfm
EC EC
qyB EFs
Ei Ei
EFm EFs EFm qyB
d EV d EV
p-type n-type
metal oxide semiconductor metal oxide semiconductor

Figure 15.27. Energy band diagrams of ideal p-type and n-type MOS structures.

inversion
V 0 EC
EFm EC V 0 Ei
EC V 0
Ei EFs
Ei EFs EV
EFs EV
EV EFm
EFm
(a) (b) (c)
Figure 15.28. Energy band diagrams for an ideal p-type MOS structure under bias.
(a) The band structure with the gate at negative voltage, termed accumulation. (b)
The band structure with the gate at positive voltage, termed depletion. (c) The band
structure with the gate at a large positive voltage, termed inversion.

a depletion region to form at the oxide-semiconductor interface. The depletion depth W is a function of
the voltage and also the background doping concentration of the semiconductor substrate, where the space
charge per unit area is approximated by
Qsc = −qe NA W, (15.127)
for a p-type substrate. A similar situation occurs if a negative voltage is applied to an n-type substrate so
that
Qsc = qe ND W. (15.128)
If a radiation event produces electron-hole pairs in the semiconductor, the electrons accumulate in the
potential well at the interface. With a readout contact adjacent to the oxide layer, this charge can be
removed and measured, an ability that underlies the operation of the charge-coupled device discussed in the
next chapter.
As the positive voltage is increased further, the depletion region continues to increase until the intrinsic
Fermi energy Ei is bent down at the interface to the same value of the Fermi energy EFs in the semiconductor.
Increasing the voltage even more causes Ei to cross over EFs and the Fermi energy approaches the conduction
band. The minority electron concentration increases at the interface as
EFs − Ei
np = ni exp , (15.129)
kT
660 Basics of Semiconductor Detector Devices Chap. 15

and causes the p-type material to act as n-type material, an operating condition termed inversion. As the
bias is increased further, the conduction band EC eventually comes close to EFs , and the electron population
near the interface increases rapidly. Hence, the charge density confined to a narrow inversion region of width
xi directly under the oxide becomes dominated by the electron population, and not the semiconductor space
charge. Consequently, after the inversion layer is formed, additional voltage does not increase the depletion
width, but instead tends to increase the electron density that opposes the additional applied voltage. In
other words, with strong inversion, the depletion region no longer increases in width with higher voltage.
With strong inversion, the total charge per unit area becomes

Qs = −qe np xi − qe NA Wmax . (15.130)

The opposite situation occurs for an n-type substrate, namely

Qs = qe pn xi + qe ND Wmax . (15.131)

Consider the diagram of Fig. 15.26(b) under inversion. A electron rich population appears under the
oxide connecting the source and drain. Hence, charge can flow across the device while under the inversion
condition. Reduction of the voltage on the gate causes the device to return to the depletion condition,
effectively stopping the charge flow. This behavior is fundamentally how the MOS-FET operates as a
current switch.5
The maximum depletion width determines the potential at which the concentration of electrons at the
surface is equal to the space charge density of the depleted volume. Here the electrostatic potential ψ is
defined as the difference between the intrinsic Fermi energy in the semiconductor bulk (beyond the depletion
region) to that near the surface region where the bands are bent so that

qe ψ = Eibulk − Eibent . (15.132)

Hence, ψ is zero in the semiconductor bulk. The surface potential is defined as

qe ψs = Eibulk − Eisur . (15.133)

The surface electron concentration can then be represented as


qe (ψs − ψB )
nsur = ni exp , (15.134)
kT
and the surface hole population as

qe (ψB − ψs )
psur = ni exp , (15.135)
kT

in which ψB = Ei − EFs in the bulk (see Fig. 15.27). The opposite conditions exist for the n-type substrate.
The potential distribution under the oxide can be calculated from Poisson’s equation as [Sze 1981]
 x 2
ψ(x) = ψs 1 − , (15.136)
W
5 Because the inversion layer behaves as an n-type channel, this type of device is called NMOS, after the type of inversion
channel and not the substrate dopant. Similarly, a MOS device formed on an n-type substrate produces a hole-filled p-type
inversion channel, and is thus called PMOS. Transistor circuits with complementary pairs of NMOS and PMOS transistors
are called CMOS.
Sec. 15.3. Basic Semiconductor Detector Configurations 661

where the surface potential is


qe N A W 2
ψs = . (15.137)
2κs 0
The surface potential at which strong inversion appears is generally accepted as approximately equal to
2ψB or
2kT NA
ψinv  2ψB = ln , (15.138)
qe ni
for p-type substrates, and
2kT ND
ψinv  2ψB = ln , (15.139)
qe ni
for n-type substrates. Substitution of Eq. (15.138) into Eq. (15.136) yields
  1/2
4κs 0 kT NA
Wmax = ln , (15.140)
qe2 NA ni

for p-type substrates where, from Eq. (15.127),


  1/2
NA 1/2
Qsc = −qe NA W = − 4NA κs 0 kT ln = − [4qe NA κs 0 ψB ] . (15.141)
ni

Similarly, for n-type substrates


  1/2
4κs 0 kT ND
Wmax = ln , (15.142)
qe2 ND ni
and   1/2
ND 1/2
Qsc = qe ND W = 4NA κs 0 kT ln = [4qe ND κs 0 ψB ] . (15.143)
ni
Another important measure is the threshold voltage at deep inversion. Note that the potential applied
to the gate drops partially through the oxide layer. Hence, the total voltage required to reach deep inversion
includes both the voltage across the oxide Vo and the depletion region ψs , i.e., VG = Vo +ψs . The capacitance
per unit area across the oxide is defined as
κo  0
Co = , (15.144)
d
where d is the oxide thickness. Hence, the threshold voltage VT becomes
1/2
−Qsc 4d2 qe NA κs ψB
VT = + 2ψB = + 2ψB . (15.145)
Co κ2o 0

or for n-type substrates


1/2
4d2 qe ND κs ψB
VT = − − 2ψB . (15.146)
κ2o 0
There are a few important features that can be gleaned from this simple ideal example. First, the maximum
depletion region possible for a MOS structure is approximately proportional to the inverse of NA,D . Second,
the threshold voltage for deep inversion increases with substrate background dopant concentration and oxide
thickness. Third, the capacitance per unit area increases as the oxide thickness d is decreased.
662 Basics of Semiconductor Detector Devices Chap. 15

vacuum level vacuum level

qcs qfs qfs qyFB


qfm qfB Eg

EFm EC EC
qyB qfm qyB
Ei Ei
d EFs d EFs
EFm
p-type EV p-type EV
metal oxide metal oxide
semiconductor semiconductor

inversion
region
Figure 15.29. Energy band diagram for a more realistic p-type MOS structure. (left) The structure before
equilibrium and (right) after equilibrium with a constant Fermi energy level.

However, there are additional properties of a common MOS device that are important to understand
in order to use a MOS device in radiation detection applications. First, seldom are the work functions of
both the metal and semiconductor equal. Second, impurities and defects in the oxide and at the oxide-
semiconductor interface can produce space charge, which, in turn, affects the operating potentials of the
device. Consider the diagram of Fig. 15.29 for a p-type substrate MOS structure. The work function of the
metal is somewhat less than the semiconductor. As the materials are brought into contact, the bands bend
to produce a flat Fermi energy, as shown in Fig. 15.29(right). Hence, to flatten the bands, a negative voltage
must be applied to straighten the bands. This voltage is termed the flat-band voltage VF B . The flat-band
voltage must adjust for the difference in the work function (φm − φs ) and the oxide space charge (Qsc ), i.e.,
Qsc
VF B = qe (φm − φs ) + . (15.147)
Co
The operating gate voltage must be adjusted to account for the flat-band voltage as

VG = VG − VF B , (15.148)

and the threshold for the onset of deep inversion becomes

VT = VT − VF B . (15.149)

Hence, it is possible that the device is in an inversion condition at zero voltage. It should be noted that
the operating potential VG changes as Qsc changes, which is a major concern for MOS devices operated in a
radiation environment. This space charge can arise from many sources, including interface trapped charge,
fixed oxide charges, mobile ions, and trapped charges. Interface charge is a function of the semiconductor
surface type and preparation. The 100 Si surface generally has the lowest density of surface states and
is preferred over a 111 Si surface for MOS devices [Sze 1981]. Contamination of the oxide can produce a
strong electric field which moves any mobile charges. Contamination from alkali metals, such as Na+ ions,
is often a source of mobile charges. Fixed charge, usually positive, is caused by oxide defects near the oxide-
semiconductor surface and cannot be eliminated once formed. Finally, trapped charge is produced as a result
Sec. 15.3. Basic Semiconductor Detector Configurations 663

of radiation damage, usually from charged particles and x-ray irradiation. As the trapped charge increases,
the voltage required to operate the device increases, ultimately causing catastrophic failure. Dopant type
inversion can also occur in the semiconductor, especially under neutron irradiation, where transmutation
activation can change the semiconductor work function over time.

15.3.5 Ohmic Contacts


Efficient charge carrier extraction from a semiconductor detector requires ohmic-like contacts; hence, it can
be important that the metal/semiconductor interface not form a rectifying potential barrier. For instance,
metal contacts to the n and p regions of pn and pin detectors are constructed so as to be non-rectifying or
ohmic, i.e., they have a current-voltage relationship that satisfies Ohm’s Law. For “ideal” ohmic contacts, a
careful choice of metals upon a selected semiconductor can produce a non-rectifying junction. Unfortunately,
because of interface state pinning, a potential barrier is formed when almost any metal is applied to the
surface of semiconductors. To remedy this problem, degenerate doping is applied with the metal and diffused,
typically through thermal treatment, into the semiconductor. The process causes the Schottky barrier to
become extremely thin such that electrons can tunnel directly through the barrier, thereby producing a
contact with ohmic behavior.
Schottky diodes are typically constructed with one (or more) Schottky contact used as a rectifying barrier
to reduce leakage current and one (or more) opposing ohmic contact to allow more efficient carrier extraction,
thereby reducing electronic noise (see depiction in Fig. 15.19).
Ideal Ohmic Contacts
Consider the case in which the work function of vacuum level
the metal is smaller than the work function of an
n-type semiconductor, as is shown in the left-hand qfm qfs qcs
part of Fig. 15.30. In order for the Fermi energies in EC
the metal and semiconductor to align, the semicon- EFm
EFs
ductor energy bands bend downward, as shown in
Fig. 15.31. For p-type material, the metal work
EV
function must be larger than the semiconductor
work function, in which case the bands bend up-
wards, as is depicted in the right-hand portion of
Fig. 15.31.
For the n-type ohmic contact, electrons in the Figure 15.30. Energy band conditions for an ideal n-type ohmic
contact.
conduction band no longer encounter an energy
barrier when drifting into the metal contact. Similarly, the holes no longer encounter and energy bar-
rier at the metal-semiconductor interface. In both cases, the contact and resulting device have a linear
current-voltage (IV) relationship that follows Ohm’s law.
Tunneling Ohmic Contacts
As mentioned before, semiconductor surfaces typically have defects and impurity contamination. These im-
perfections may arise from the cutting and polishing processes that are usually incorporated during detector
fabrication. Although subsequent liberal surface etching can remove much of the damage, sufficient surface
damage usually remains that “pins” the energy barrier at the metal/semiconductor interface. Hence, the
above ideal model of the ohmic contacts rarely applies.
Ohmic contacts can be made, however, by introducing degenerate doping at the semiconductor surface
before or during the metal contact application, with degenerate n-type dopant levels introduced to n-type
material and degenerate p-type dopant levels introduced to p-type material. The dopant is diffused into the
surface, causing the bands to bend strongly at the interface. Although an energy barrier still appears, the
664 Basics of Semiconductor Detector Devices Chap. 15

vacuum level vacuum level

qcs qcs
qfs qfm EC
qfm qfs
EC EFs
EFm EFm
EFs EV
EV

n-type ideal ohmic contact p-type ideal ohmic contact


Figure 15.31. Energy band diagrams for ideal n-type and p-type ohmic contacts.

n+ region
n region
EC EC
EFm EFs EFm EFs
metal metal
EV EV

n-type dopant
Figure 15.32. Interface states and band conditions for a tunneling n-type ohmic contact.

EC
EC
EFs
EFm EFs EFm
EV
metal EV metal

n-type tunneling ohmic contact p-type tunneling ohmic contact


Figure 15.33. Energy band diagrams for n-type and p-type tunneling ohmic contacts.

actual barrier width is relatively small such that the charge carriers can tunnel directly through the barrier.
The result is a linear IV relationship that follows Ohm’s law. The interface states and energy bands for
tunneling ohmic contacts are shown in Fig. 15.32 and Fig. 15.33, respectively.
The degenerate doping may be applied by traditional methods, such as ion implantation or thermal
diffusion. Often a metal eutectic, partially composed of an element that is a dopant in the semiconductor,
is applied to the surface and annealed so that the dopants become active in the semiconductor surface.
Examples include AuGeNi annealed into n-type GaAs and AuZn annealed into p-type GaAs. Here Ge is an
Sec. 15.3. Basic Semiconductor Detector Configurations 665

n-type dopant and Zn is a p-type dopant. Often a chemical reaction may produce the desired effects, such
as occurs in the application of AuCl3 to p-type CdTe or CdZnTe. The AuCl3 reacts with the Cd, displacing
it, and deposits Au in the material, which acts as a p-type dopant.

15.3.6 Series Resistance and Space Charge Effects


Wide band-gap semiconductors are of interest because many can be operated at room temperature without
the complications of cryogenic or mechanical cooling. Unfortunately, all of these room temperature semi-
conductors are compound materials,6 and consequently, these semiconductors typically have low electrical
resistivity from residual background impurities that are difficult to remove, or possess high concentrations
of native defects that act as charge carrier donors or acceptors. The resistivity of these interesting materials
can be significantly increased by clever additions of deep energy levels. These energy levels can be added
through the purposeful introduction of deep dopant impurities or native defect states. The unintentional
introduction of impurities and trapping centers and the purposeful introduction of compensating centers,
work together to reduce the free charge carrier concentration, and thereby increase the resistivity of the
semiconductor (as demonstrated in Chapter 12). These traps and compensating centers can produce space
charge in the semiconductor when filled (or emptied, depending on type). The combined effect of series
resistance and space charge alters the forward bias current characteristic in a semiconductor device.
However, the traps can cause issues with the internal electric field within the device, under either forward
or reverse bias. Under forward bias, the high series resistance of the detector causes a reduction in the
observed current, namely " #
qe (V − JRA)
J = Js exp −1 , (15.150)
kT
where Js is the saturation current density, V is the applied voltage, J is the current density, R is the diode
forward resistance, and A is the diode effective area. As the resistance R in Eq. (15.150) is increased, the
amount of voltage at the rectifying junction decreases, which causes a decrease in the observed current
(Fig. 15.34). The result is a gradually rising forward current characteristic, often modeled with a corrective
“ideality factor” n̆ as " #
qe V
J ≈ Js exp −1 , (15.151)
n̆kT
and the subsequent results are shown in Fig. 15.35. Rhoderick and Williams [1988] point out that the oft-
used Eq. (15.151) in the literature is an incorrect form, and that the more correct form should actually be
Eq. (15.112), mainly because of changes in the rectifying barrier physics. However, additional problems from
series resistance and space charge limitations render that argument less effective, mainly because forward bias
currents are controlled by other mechanisms than just the contact barrier height. Regardless, Eq. (15.151)
is an approximation of the observed case.
The general case for electron current flow in an ideal insulating medium is approached with the current
density Eq. (15.67). Consider the case in which electrical contacts are applied to an insulating slab, across
which is applied a voltage V0 . For general conditions, drift current is substantially higher than the diffusion
current. Hence, Eq. (15.67) reduces to
J  qe μn n(x)E(x). (15.152)
If n(x) is uniform, then from Poisson’s equation
 
J
E(x)dE = dx, (15.153)
μn s

6 Diamond is an exception, but is inadequate as a gamma-ray detector because of the low Z number.
666 Basics of Semiconductor Detector Devices Chap. 15

Figure 15.34. The ratio J/Js plotted as a function of series resistance for the case
Js = 1 nA cm−2 .

or
1/2
2Jx
E(x) = +C , (15.154)
μn s
where C is an integration constant. For the simplified case, it is assumed that the electric field is zero at the
cathode (x = 0) [Wright 1959], hence C = 0. The voltage drop across the insulating slab is
 W  W 1/2 1/2
2Jx 2 2J
V = E(x)dx = dx = W 3/2 , (15.155)
0 0 μn s 3 μn s

where W is the slab thickness. Substitution of i = JA and rearrangement of the terms in Eq. (15.155) yields
the current
9 μn s AV 2
i= , (15.156)
8 W3
where A is the effective contact area. Eq. (15.156) is known as Child’s Law for solids, as developed by Mott
and Gurney [1948].7
The forward current characteristic can also be affected by space charge buildup from the injected current.
As the injected current is increased by the applied bias, the traps in the semiconductor material become
filled at a rate high enough to produce a net space charge at steady state. More traps are filled as the
forward voltage is increased, a case studied in detail by Rose [1963], Tredgold [1966], Lampert [1956], and
Lampert and Mark [1970]. Consider that case in which a semiconductor has a trap density NT . The voltage
at which all traps are filled is similar to the one-sided depletion approximation, i.e., the trap-filled-limit

7 Eq. (15.156) is also known as the “trap-free square law” or the “Mott-Gurney square law”.
Sec. 15.3. Basic Semiconductor Detector Configurations 667

Figure 15.35. The ratio J/Js plotted as a function of the ideality factor n.

voltage (VT F L ) is [Wright 1959]


qe N T W 2
VT F L = . (15.157)
2s
Below VT F L , the current is reduced by the trapping
effect, which can be shown to be an alteration of
Eq. (15.156) [Lampert and Mark 1970]
  
 

9 μn s θAV 2
i= (15.158)
8 W3
  
where θ is the fraction of injected charge that is   


untrapped and remains available for current flow.


Eq. (15.158) is referred to as the modified Child’s Law.
Three regions can usually be observed for space charge
limited solids, namely, the ohmic region at very low volt-     
ages, the modified Child’s Law region (Eq. (15.158)),
and the Child’s Law region (Eq. (15.156)). At low volt-   
ages, the current appears to have an ohmic response,
Figure 15.36. Rectifying behavior of space charge limited
i.e. i ∝ V . As the voltage is increased, traps begin to conduction through a solid.
fill and produce a space charge region, which affects the
electric field and increases current flow (i ∝ V 2 ). At VT F L the traps are filled and an abrupt increase
appears in the current characteristic from Eq. (15.158) to Eq. (15.156), above which is the full Child’s Law
region (see Fig. 15.36). This rectifying behavior is due to the overall trap density of the semiconductor (or
semi-insulator) rather than a contact barrier or junction chemical potential.
668 Basics of Semiconductor Detector Devices Chap. 15

Note that one of the assumptions with Eq. (15.156) and Eq. (15.158) is that the charge carrier speed is
proportional to μE, thus yielding one of the voltage terms. At high electric fields the charge carrier speeds
saturate and it becomes possible that i ∝ V rather than V 2 .

15.3.7 Resistive and Photoconductive Devices


There are detectors that operate without rectifying contacts, namely resistive and photoconductive detectors.
Resistive detectors have such high resistivity that rectifying barriers are not needed to reduce the leakage
current, and photoconductive devices use efficient charge injection to produce photoconductive gain.
Resistive Devices
Semiconductor detectors fabricated from wide band-gap materials (generally > 1.6 eV) have material re-
sistivities high enough to reduce leakage currents to low levels, and, as a result, do not require rectifying
contacts to suppress leakage currents. The devices typically have ohmic contacts as electrodes to prevent
rectification and the formation of space-charge regions (which limits the active region volume). Radiation
interactions in the detectors create electron-hole pairs that are swept out of the detectors by an applied
electric field. The high resistivity of the device ensures that the leakage current is significantly lower than
the current produced by radiation interactions in the device. For example, the current from a common
5-mm (width) × 10-mm × 10-mm CdZnTe detector, with a 1.62-eV band gap and electron mobility of 1350
cm2 V−1 s−1 , has a resistivity of 1011 Ω cm, so that the detector has a resistance of 5 × 1010 Ω. At a bias
of 500 volts, the electric field is 103 V cm−1 with a leakage current of 10−8 amps. The electron population
is found from Eq. (15.152), from which the steady-state charge population is found to be 4.6 × 104 cm−3 .
Given the volume, the steady-state electron charge population in motion for the detector is 2.3 × 104 cm−3 .
The average ionization energy of CdZnTe is 5 eV; hence, a 662-keV gamma ray produces approximately
1.32 × 105 electron-hole pairs, thereby increasing the total electron population in the device, momentarily,
by 5.74 times. Should the resistivity decrease, the leakage current would add more to the output, whereas an
increase in resistivity would decrease the influence of leakage current. Notably, energy resolution degrades
from fluctuations in the leakage current, which generally increases as the leakage current increases.
Photoconductive Devices
There is a unique class of semiconductor detectors known as photoconductors. To understand how these
devices work, consider a semiconductor to which ohmic contacts are affixed that prevent the creation of a
blocking barrier and a space-charge region. Such a device is in essence an ohmic resistor. From Eq. (12.90)
it is seen that the resistivity of a semiconducting material is inversely proportional to the free carrier con-
centration. Further, the free carrier concentrations are affected by thermal changes and impurity atoms.
Free carriers are also produced in the semiconductor by gamma-ray interactions. For example, fast
electrons are produced as photoelectrons, Compton recoil electrons and, for photons of sufficient energy, as
pair production electrons. These fast electrons create many electron-hole pairs as they slow down, producing
a small localized charge cloud. Thus, for a single radiation event in a conventional diode detector, the local
conductivity is changed spontaneously; however, the small charge cloud is surrounded by higher resistivity
material on all sides. Further, the charge cloud is dissipated rapidly by the applied voltage.
Suppose, however, the semiconductor block is saturated with a radiation pulse, consisting of a huge
number of radiation quanta, such that electron-hole pairs are evenly distributed throughout the crystal bulk.
Now, the conductivity of the entire semiconductor block increases because of the large and uniform injection
of free carriers throughout the semiconductor crystal. Thus, with a constant applied voltage, the current
flowing through the device must increase. After the pulse, the current continues to flow, if the ohmic contacts
are well-fabricated, because every electron exiting the device at the anode is replaced by another electron
injected at the cathode. This photocurrent continues to flow, decaying away as a function of the free charge
carriers lifetimes.
Sec. 15.3. Basic Semiconductor Detector Configurations 669

A photoconductor consists of a semiconductor material upon which ohmic contacts have been applied.
For pure (intrinsic) semiconductors, the conductivity can be described by

σ = ρ−1 = qe (nμn + pμp ), (15.159)

where qe is the unit electronic charge, n is the negative electron population, p is the positive “hole” population,
and μ is the mobility of either electrons or holes. Photons interacting with the semiconductor excite electrons
into the conduction band and, thus, serve to increase n, p, and the conductivity. The resistance of the material
is described by
ρL L
R= = , (15.160)
A σA
where L is the effective device length and A is the effective cross sectional area of the device. Hence, the
observed current is
σAV
I= = σAE = qe AE(nμn + pμp ), (15.161)
L
where V is the applied voltage and E is the electric field. Note that the photocurrent is a direct function of
the charge carrier densities n and p. Suppose that Δn the increase in the electron charge carriers produced
by an impulse of light. Hence, n(t) = no + Δn exp(−t/τ ), where n0 is the electron charge carrier population
without light, i.e., the dark current. These charge carriers recombine or become trapped, so that charge
carriers have a mean lifetime of τ . Under steady-state irradiation, free charge carriers that recombine are
regenerated at the same rate, hence the generation rate per unit volume becomes G = n/τ or

n 1 qe ηQ Po
= , (15.162)
τ AL hν
where Po is the optical power density and ηQ is the quantum efficiency.8 The electron current contribution
is found by substituting Eq. (15.161) into Eq. (15.160) to obtain

(μn τn + μp τp )E qe ηQ Po
I = In + Ip = . (15.163)
L hν
The primary photocurrent is described by

qe ηQ Po
Iprim = , (15.164)

which is the contribution to the current from the initial photoelectric excitation. However, because the
resistivity changes with irradiation, charge carriers are injected into one contact as they exit the opposite
contact, as required by Ohm’s law. Hence, the photocurrent gain is [Bube 1960]

I (μn τn + μp τp )E (vn τn + vp τp ) τn τp
MPC = = = = + , (15.165)
Iprim L L tn tp

where tn and tp are the transit times across the device for electrons and holes, respectively. For a single flash
of light, from a scintillator for instance, the current is described by

I = qe AE(μn (no + Δne−t/τn ) + μp (po + Δpe−t/τp )). (15.166)

8 Here ηQ is defined as the number of electron-hole pairs excited per photon.


670 Basics of Semiconductor Detector Devices Chap. 15

The current is largely affected by the excited charge carrier populations Δn and Δp, which eventually return
to the dark current density of n0 and p0 . If the photocurrent is primarily from band to band transitions
with n0 = p0 , then Eq. (15.166) reduces to
I = qe AE(no + Δne−t/τn )(μn + μp ). (15.167)
The gain for such a device is dominated by the charge carrier lifetimes. Hence, high speed devices require
short lifetimes, whereas high gain devices require long lifetimes. Further, the fluctuation in current can be
problematic and leads to poor energy resolution. Consequently, photoconductors are usually not the light
sensing device of choice for scintillation detector spectroscopy.
For a planar device, Eq. (15.167) can be rewritten as
qe V A
I(t) = (no + Δne−t/τn )(μn + μp ). (15.168)
L
This result is important. First, the current decays away as a function of the free charge carrier lifetime, so
that the current can continue to flow even after the primary charge carriers produced in the semiconductor
reach the electrodes. Second, the duration of the detector current pulse can be tailored by changing the
lifetime of the free charge carriers. High speed photoconductive radiation detectors can be manufactured
by purposely adding lifetime shortening dopants, or by shortening the lifetimes with intentional radiation
damage. These detectors are ideal for fast timing measurements of large radiation bursts.

15.3.8 Photon Drag Detectors


A special type of photoconductor is the photon drag detector, which operates by sensing momentum changes
of free charge carriers. These special photoconductive detectors are used primarily to measure high intensity
beams of infrared radiation, such as laser emissions. Photon drag detectors consist of a semiconductor bar,
generally cylindrical, around which ring electrodes have been fashioned near the ends [Gibson and Kimmitt
1980]. The semiconductor is selected such that the band-gap energy is greater than the photon energy under
investigation, thereby allowing a large fraction of photons to pass directly through the semiconductor without
being absorbed. For instance, initial photon drag experiments were conducted with p-type Ge (Eg  0.7
eV) for λ = 10.6 μm (0.117 eV) light [Grinberg 1970; Danishevskiĭ et al. 1970; Gibson et al. 1970].
When photons and electrons interact, the electrons can gain energy and momentum. Consider a beam of
photons having a cross section A impinging lengthwise upon a semiconductor cylinder of length L0 . These
electrons, having gained some momentum, acquire an ordered motion in the direction of the light propagation
and a momentum transfer rate of
αW ne−αL
M= , (15.169)
Ac
where c is the light speed, W is power in watts, n is the index of refraction, α is the optical absorption
coefficient in cm−1 , L is the location along the semiconductor length. The motion of charge carriers produces
an opposing electric field
αW ne−αL
qe E = , (15.170)
nc Ac
where nc is the majority charge carrier density. If the majority carriers are holes, then the electric field
polarity is reversed. Hence, momentum is transferred to holes in the valence band. Integration of Eq. (15.170)
over the device length gives the resulting voltage per unit power illuminating the detector. After reflection
at both ends of the device are included [Gibson et al. 1970], the voltage per unit power is
V −ρμn(1 − R)(1 − e−αL0 )
= , (15.171)
W Ac(1 + Re−αL0 )
Sec. 15.4. Measurements of Semiconductor Detector Properties 671

where R is the semiconductor reflection coefficient (two facets), ρ is the semiconductor resistivity, μ is the
majority charge carrier mobility, and L0 is the length of the sample. For heavily doped samples, the product
αL0 is relatively large, and Eq. (15.171) reduces to

V −ρμn(1 − R)
≈ , (15.172)
W Ac

Hence, the photon drag detector operates as an infrared detector in which radiation passes through a doped
semiconductor crystal, creating a measurable voltage drop associated with the photon beam intensity. Overall
the effect is small and photon drag detectors are generally only useful for the detection of high fluxes of sub-
band-gap radiation, such as from an infrared laser source. Numerous semiconductors have been investigated
for these detectors, including Ge, Si, Te, GaAs, GaP, an InAs, as described in the literature [Gibson and
Kimmitt 1980]. Photon drag detectors can be acquired through several commercial manufacturers of light
sensors, the most common one composed of p-type Ge.

15.4 Measurements of Semiconductor Detector Properties


Synthesis and development of semiconductor materials and semiconductor detectors requires characterization
of certain properties to better understand expected performance of a detector. For instance, the energy
resolution from a semiconductor material is strongly dependent upon the product of the charge carrier
mobility and the charge carrier mean free drift time, commonly referred to as the μτ product. Analysis
of semiconductor detectors is often accomplished through measurements of fundamental properties, which
include measurements of current, capacitance, the μτ product, electrical contact resistance, and charge
carrier trapping. There are many excellent books devoted to this topic (see for examples [Look 1989; and
Schroder 1990]). Only the more fundamental characterization methods are briefly described here.

15.4.1 IV Measurements
The current-voltage characteristic, or IV characteristic, is a fundamental property that yields leakage cur-
rents, normally under reverse bias. The quality of a blocking contact is generally revealed by the overall
leakage current density that is observed. The measurement is typically performed with a probe station,
manual or automated, that applies a voltage across a junction device and measures that resulting current.
Common commercial systems allow reverse (negative) or forward (positive) voltage to be applied across a
junction, automated with incrementally increasing steps. Many systems have built-in safety circuits that
allow the establishment of a “compliance” limit to the measured current, beyond which the voltage is turned
off.
The measurement is simple and the logarithm of the absolute value of the current is typically plotted
against the applied voltage on a linear voltage scale showing both the forward and reverse currents. Recall
the thermionic current for a pn junction is (see Eq. (15.75) and also Eq. (15.112))

  
 qe V 
I = Is exp − 1  . (15.173)
n̆kT

The resulting plot, shown in Fig. 15.37, is useful in (a) revealing the reverse leakage current and diode quality,
and (b) issues with series resistance and space-charge limitations for the forward bias characteristic.
672 Basics of Semiconductor Detector Devices Chap. 15

Figure 15.37. Conventional IV method of plotting the iv Figure 15.38. The IV plotting method proposed by Mis-
characteristic of a diode. The device is a 1 cm2 Schottky sous and Rhoderick [1986]. The plot yields n = 1.0183 and
barrier Si detector. is = 3.084 nA.

Missous and Rhoderick [1986] propose another method, based on Eq. (15.112), that yields additional
information about n. In this method a plot of the quantity
⎛ ⎞
⎜ I ⎟
ln ⎜

⎟, (15.174)
−qe V ⎠
1 − exp
kT

versus the applied voltage V gives a linear plot of the IV characteristic at all values of V , including those
values of V < 3kT /qe , as shown in Fig. 15.38. From Eq. (15.112), the following relationship is obtained

qe V
ln(Is ) + ∝ V. (15.175)
n̆kT

The slope of the resulting graph yields the value of n, but primarily from the forward current. Also possible
is a determination of Is (or Js ) at the V = 0 intercept. From the relationship of Eq. (15.108), these mea-
surements can yield information on the rectifying barrier height. Note that deviation from linearity can still
occur from space charge limited current under forward bias, and charge carrier trapping and recombination
can also cause distortions for reverse bias currents.
Sec. 15.4. Measurements of Semiconductor Detector Properties 673

15.4.2 CV Measurements
The capacitance-voltage (or CV ) characteristic can be used to determine a semiconductor doping concen-
tration or the depletion width as a function of voltage for a junction device. The original CV measurement
method was developed by Hilibrand and Gold [1960] for a parallel plate design. Recall the relationships

dQ
C =− , (15.176)
dV
in which the differential change in charge is negative from electron contributions, and

dQ = −qe A|ND (W ) − NA (W )|dW, (15.177)

where qe is the unit charge, A is the device area, |ND (W ) − NA (W )| is the net doping concentration as a
function of depletion width W , and W is the depletion width. From these two results
dQ dW dW
C =− = qe A|ND (W ) − NA (W )| = qe ANb . (15.178)
dV dV dV
The general assumption for a planar device is that the capacitance is a function of the depletion layer width,
i.e.,
s A
C= . (15.179)
W
Substitution of Eq. (15.59) or Eq. (15.103) into Eq. (15.179) yields,

qe s Nb A2
C2 = . (15.180)
2(Vbi − V )
This result can be rearranged to give

1 qe s Nb A2
V =− + Vbi . (15.181)
C2 2
The result of Eq. (15.181) is rather impor-
tant. A plot of 1/C 2 versus the applied volt-
age V yields the semiconductor doping con-
centration and the built-in potential Vbi (see
Fig. 15.39). Further, knowledge of A and C
determines the active region width W from
Eq. (15.179). Muller and Kamins [1986] point
out that the value determined for Nb is gener-
ally accurate, although the value determined for
Vbi can be have significant error.9 The slope of
1/C 2 can be determined by simple differentia-
tion, namely
Figure 15.39. The two types of capacitance plots most often used
d 1 d 2(Vbi − V ) −2 in semiconductor radiation detector analysis. Shown is the case for a
= = . Si Schottky diode 1 cm2 area, Nb = 5.5 × 1013 cm−3 , and Vbi = 0.37
dV C2 dV qe s Nb A2 qe s Nb A2
volts.
(15.182)

9A small change in the slope causes a large change in the intercept value Vbi .
674 Basics of Semiconductor Detector Devices Chap. 15

A common method of determining full depletion for a junction diode is to observe the voltage at which the
CV characteristic curve stops changing and reaches a constant value.
The capacitance can be measured with a CV system consisting of an applied simultaneous DC voltage
and a smaller AC voltage through a capacitance bridge, and yields the general relationship for current
V V
I= = = jωV C, (15.183)
Z (jωC)−1

where j is −1, ω is the modulation frequency, Z is the device impedance, V is the applied voltage, and
C is the capacitance. Typically, the modulation frequencies range between 10 kHz to 10 MHz. These
measurements work well for the smaller band-gap semiconductors such as Ge and Si. However, problems
can arise with the larger band-gap semiconductors having band energies above 1.2 eV.
For wide band-gap semiconductors, the series resistance in the substrate region can become problematic
and yield incorrect results. The simple assumption of Eq. (15.183) is that the impedance of the diode is
dominated by the depletion region capacitance and the undepleted substrate region capacitance is essentially
shorted by the semiconductor conductivity. However, there is a parallel resistance with the depletion layer
capacitance, which is also true for the undepleted substrate. Hence, there is a series resistance R that can
confuse the capacitance measurement

V Rω 2 C 2 jωC
I= =V + . (15.184)
R + (jωC)−1 1 + (ωRC) 2 1 + (ωRC)2

The true capacitance can be determined from the measured capacitance Cm by [Look 1989]

C
Cm = . (15.185)
1 + (ωRC)2

The actual doping concentration, corrected for series resistance, is [Wiley 1975]
3
Cm
|ND (W ) − NA (W )| = − , (15.186)
qe s A2 sin φ[dCm /dV − 2Cm (dφ/dV ) cot φ]
4

where φ is the phase angle obtained from tan φ = (ωRC)−1 . If the product ωRC  0.2, then the measured
doping profile is distorted [Look 1989].
If the substrate is a semi-insulator, the result can become unreliable. Consider the small signal model
of a detector in (Fig. 15.40), simplified by showing a depletion region, a substrate region, and the electrical
contacts. If it is assumed that the electrical contacts are well made, then the resistances short out the
contact capacitance, rendering their contributions minor. However, that is not the case for the substrate
region, where R is significant and cannot be ignored.
Hence, the simple small signal circuit has an impedance

RD RS
Z= + , (15.187)
1 + jωRD CD 1 + jωRS CS

where the D and S subscripts indicate the depletion region and substrate regions, respectively. For high
modulation frequencies ω and high substrate resistivities, the impedance takes the form [McGregor and
Kammeraad 1995]
ρ(WD + WS )
Z≈ , (15.188)
A(jωρs + 1)
Sec. 15.4. Measurements of Semiconductor Detector Properties 675

DETECTOR
RC1 RD RS RC2

A
CA

CC1 CD CS CC2
RL

Figure 15.40. Small signal equivalent circuit model of a semiconductor detector.


[Adapted from Walter 1960].

where ρ is the substrate resistivity, WD is the depletion layer width, and WS is the substrate layer width.
The current is approximated by
1
I=V + jωCT , (15.189)
(RD + RS )
where CT is the series combination of CD and CS , representing the total capacitance between the electrical
contacts. This important result shows that (1) sufficiently high frequencies and (2) sufficiently high semi-
conductor resistivities reduce the measured capacitance to CT . In either case, the observed capacitance does
not change with voltage, erroneously misleading the measurement to indicate that the device active region10
extends completely across the device, when in fact it does not [McGregor and Kammeraad 1995].

15.4.3 Measurement of Contact Resistance


Contact resistance is another fundamental property used as a quality metric for semiconductor detectors.
The resistance of a blocking contact gives a measure of the rectification quality, while the resistance of an
ohmic contact is used as a measure of conductance quality. The higher the blocking contact resistance,
above the natural resistivity of the semiconductor, the more the leakage current is reduced. The lower
the resistance of an ohmic contact, the smaller is the voltage drop at the contact so that there is better
charge carrier collection and lower shot noise. IV measurements do pro-
vide a good first measurement of the rectifying behavior of a semiconduc- RT1 RT2
tor diode detector, but do not disclose the contact resistance RC . There
are many methods to measure this contact resistance (see Look [1989] W C1 C2 C3
and; Schroder [1990]), a few of which are described here.
The transmission line model (TLM), based on the pattern of L l1 l2
Fig. 15.41, is a simple three-terminal design with which the contact re-
sistance can be estimated. The total resistance from one contact to an Figure 15.41. The transmission line
adjacent contact is model pattern, with ohmic contacts of
rs li width W , length L, and gap distances
RT i = , (15.190) of l1 and l2 . The contacts, labeled C1 ,
W + 2Rc C2 , and C3 , are presumed identical.
where rs is the sheet resistance,11 W is the contact width, Rc is the contact resistance, and li is the distance
between the contact edges. The measurement is made by placing a voltage across contacts C1 and C2 to

10 The substitute use of ‘active region’ is much more accurate than the term ‘depletion region’. The active region describes the
region in a detector where the electric field is high enough to drift the charges, whereas the depletion region describes the
region where the semiconductor is devoid of charge carriers. Because semi-insulating semiconductors, such as GaAs and CdTe,
are already devoid of charge carriers, the description ‘depletion region’ has less meaning than ‘active region’.
11 The units for sheet resistance are Ω/, meaning that any square of semiconductor surface yields the very same resistance. For

instance, the sheet resistance of a 1 cm × 1 cm of semiconductor square surface is the same as a 2 cm × 2 cm square surface.
676 Basics of Semiconductor Detector Devices Chap. 15

yield a current of I1 , followed by a second measurement across C2 and C3 to yield I2 . The total resistance
for either measurement is simply RT i = V /Ii . The two equations formed from this pattern are solved to
yield the contact resistance
RT 1 l2 − RT 2 l1
Rc = . (15.191)
2(l2 − l1 )
The transmission line model is simple in application, but does have accuracy problems. Errors in the
measured distances li can lead to measurement inaccuracy. Also, from Eq. (15.191), the difference between
two large numbers, combined with small contact resistances, can lead to an inaccurate determination of Rc .
The transfer length model (unfortunately also termed TLM)
is a popular method used to test the specific contact resistance l1 l2 l3 l4
of an ohmic contact. The method consists of placing consecutive
planar contacts upon a semiconductor surface and performing W C C2 C3 C4 C5
1
a series of current measurements. Consider the pattern shown
in Fig. 15.42 that has a series of identical contacts, labeled C1
L
through C5 , each with a width W and length L, placed apart
at increasing spacings. A resistance measurement is made by Figure 15.42. A common TLM pattern, with
placing a known voltage across two contacts and measuring the ohmic contacts of width W , length L, and gap
resulting current. The total resistance is distances of l1 , l2 , l3 , and l4 . The diagram de-
picts gap distances of increasing integer values,
li i.e., l4 = 4l1 .
RT = 2Rc + rs , (15.192)
W
where Rc is the contact resistance of a single contact, rs is the RT
sheet resistance between the contacts, and li is the distance be-
tween the contacts. This measurement is repeated for the four slope = rs/W
pairs of contacts shown in Fig. 15.42. The total resistance RT
(where RT = V /I) can be plotted against the intercontact dis-
tances li , and noting that Eq. (15.192) is a linear equation, the 2Rc
y intercept yields the value of 2Rc as shown in Fig. 15.43. The
x intercept is a function of the transfer length, defined as
l
2W Rc
2LT = . (15.193) -2WRc 0 l1 l2 l3 l4
rs rs
Three important values are derived from this transfer length Figure 15.43. The measured resistance as a
method, namely, Rc , rs , and the sheet resistance Rs = rs /W . function of the distance li between the ohmic con-
This method is one of the most commonly used techniques to tacts, showing the method used to find Rc .
measure the quality of an ohmic contact, but does have a few potential problems. First, this method is based
on the assumption that current flows uniformly from the contacts when, in reality, the current actually flows
between the closest edges [Look 1989]. This non-uniform current is termed current crowding. To correct for
current crowding, Look [1989] shows that the contact resistance is better described by

Rs ρc
Rc = coth (kL), (15.194)
W
where ρc is the specific contact resistivity under the metal-semiconductor interface, Rs is the sheet resistance
under the contact, L is the contact length, and k 2 = Rs /ρc . If kL  2, then ρc is well approximated by

W 2 Rc2
ρc  . (15.195)
Rs
Sec. 15.4. Measurements of Semiconductor Detector Properties 677

Note that it is assumed here that rs and Rs are interchangeable, an assumption that may not necessarily
be true. During contact processing and development, it is possible to alter the material sheet resistance such
that rs = Rs . The inclusion of effects from the end resistance can compensate for errors introduced when rs
and Rs are different. This compensation is made by either placing a guard ring around the TLM structure,
or (originally) by placing an extra contact Ce to the left of C1 (in Fig. 15.42) at distance L [Reeves and
Harrison 1982]. This extra end resistance can be found by measuring the voltage at Ce while applying a bias
between the C1 and C2 . Hence, the end resistance is [Look 1989]
V (Ce ) − V (C1 ) Rc Rc
Re = = =  , (15.196)
I cosh (kL) cosh(L Rs /ρc )
where I is the measured current. Here the actual value of Rs is found from the ratio
Rc 
= cosh (kL) = cosh(L Rs /ρc ). (15.197)
Re
Reeves and Harrison [1982] show that the difference between Rs and rs can be significant, with examples of
GaAs having a rs /Rs ratio of 19.55 and Si having rs /Rs ratio of 4.88. Issues with end resistance have been
addressed with a circular transmission line model proposed by Reeves [1980], in which a circular “bull’s eye”
pattern takes the place of the TLM pattern of Fig. 15.41. The method employs Bessel function solutions
and requires careful design considerations for the method to converge on a solution.
There is another difficulty encountered with many of the high-resistivity semiconductors, such as SI-GaAs,
CdTe, CdZnTe, and HgI2 . The substrate resistance is such a dominant factor that determining the contact
resistance can be statistically challenging. One can observe from Eq. (15.192) that if the total resistance
measured RT is large, then the error associated with a small change in the slope rs /W produces a large
variance in the transfer length. Hence, the error associated with the measurement of rs becomes large. To
reduce this error, often a contact scheme is tested on a conductive semiconductor substrate and then applied
to a semi-insulating substrate of the same type of material. However, the actual substrate resistance can
make a significant contribution to the contact resistance and lead to an incorrect result.
The chemical compatibility of electrical contacts can also be a major issue, especially with the softer
high-Z semiconductors such as HgI2 and TlBr. For instance, there are only a few conductive materials that
can be used on HgI2 that do not destructively react with the compound, namely, carbon, Pd, and Pt. Gold
rapidly diffuses in Si and, thus, produces a deep acceptor. Aluminum with gold produces a purple corrosion
(the “purple plague” - AuAl2 ) on GaAs. Hence, some amount of caution should be exercised when deciding
upon the contact material.
Finally, there are some semi-conductors used for radiation detectors with band gaps exceeding 2 eV.
Hence, they are better classified as semi-insulators. Examples include HgI2 , PbI2 , TlBr, and SiC. Contact
formation to these materials need not be rectifying, mainly because the intrinsic resistivity is sufficient to
reduce the leakage current to manageable levels. Hence, additional resistance from electrical contacts is less
of a problem, although poor contact formation may cause capacitance issues that create multiple energy
peaks in a pulse height spectrum.

15.4.4 Measurement of Resistivity


A fundamental property of a semiconductor is its resistivity, i.e.,
1
ρ= . (15.198)
qe (μe n + μh p)
Perhaps the simplest method of measuring resistivity is to place ohmic contacts on opposite ends of a
semiconductor bar of length L, followed by a measurement of the current (I) resulting from voltage (V )
678 Basics of Semiconductor Detector Devices Chap. 15

_ _
+ +
I V I I V I

t
W
s s s s s s

D L

Figure 15.44. Geometries for four-point probe measurements on circular and rectangular samples.

applied across the bar. If the area of each end is A, then the current density is
I V
= Jn + Jp = (qe nμn + qe μh p), (15.199)
A L
or
VA
. ρ= (15.200)
IL
Usually a semiconductor is dominated by one of the charge carriers, previously named the majority carrier.
Hence, the resistivity is usually due to n-type or p-type charge carrier conduction.
A common method of measuring resistivity is with a four-point probe. The system has four equally
spaced point probes, arranged in a straight line, that are brought into contact with a semiconductor surface
(see Fig. 15.44). The spacing between each probe is denoted by s. A current is supplied to the outermost
probes with a constant current source and the resulting voltage is measured between the two inner most
probes. For a thin semiconductor sample in which the thickness under investigation is much smaller than
the lateral dimensions of length L and width W , the sheet resistance is given by [Sze 1981]
π V V
rs = K = 4.5324 K. (15.201)
ln(2) I I
where K is a geometric correction factor. The volume resistivity is determined from
ρ = rs t. (15.202)
Schroder [1990] points out that geometric correction factors have been calculated by many researchers using a
variety of techniques. However, all reduce the correction factor to three important components, K = f1 f2 f3 .
The correction factor f1 corrects for differences with the sample thickness, f2 corrects for the lateral sample
dimensions, and f3 corrects for the location of the probes with respect to the sample edges. If the sample
width W is much larger than the probe spacing (W s), then Eq. (15.202) reduces to
Vt
ρ = 4.5324 , (15.203)
I
where t is the sample thickness.
For thinner samples of smaller widths W , the proper corrections must be applied. The factor f1 addresses
corrections for finite thickness t, and is given by
ln(2)
f1a =  , (15.204)
sinh(t/s)
ln
sinh(t/2s)
Sec. 15.4. Measurements of Semiconductor Detector Properties 679

if the bottom underlayer is an insulator and by


ln(2)
f1b =  , (15.205)
cosh(t/s)
ln
cosh(t/2s)
if the bottom underlayer is a conductor. The limiting values are found for t  s as
Vt
f1a ≈ 1 and ρ ≈ 4.5324 f2 , (15.206)
I
8 s2 8π s2 V
f1b ≈ ln(2) and ρ≈ f2 , (15.207)
3 t2 3 t I
and for t s as
s V
f1a = f1b ≈ 2 ln(2) and ρ ≈ 2πs f2 . (15.208)
t I
The factor f2 addresses corrections for a finite width W . Smits [1958] calculated and published a table of
these values as πf2 / ln(2) for rectangular and circular samples. The correction f2 is plotted in Fig. 15.45 for
values D/s and W/s between 1 and 40. As W/s becomes large, f2 approaches unity. The third correction fac-
tor has four possible expressions, depending on whether the probes are near a conducting or non-conducting
boundary [Valdes 1954], and also depending upon the orientation of the probes with that boundary. Plotted
in Fig. 15.46 are corrections factors for f3 for both conducting and non-conducting boundaries, according to
the probe orientation and distance-to-spacing ratio d/s. Note that in all cases f3 approaches unity provided
that the probe is at least 3s distance away from the sample edge.

15.4.5 Measurement of Charge Carrier Mobility


Recall that the mobility of an extrinsic semiconductor is
1
μe = for n-type material, (15.209)
|qe |ρe n
1
μh = for p-type material. (15.210)
|qe |ρh p
This result shows that the charge carrier mobility can be found by measuring the carrier concentration and
resistivity. The carrier concentration is commonly measured using the Hall effect, named after E.H. Hall
[1879] who discovered the effect. Hall discovered that a magnetic field applied to a material perpendicular to
a current flowing through the same material induces a voltage perpendicular to both the magnetic field and
current. Putley [1968] devotes a textbook to the study of this effect. Consider the block of semiconductor
material depicted in Fig. 15.47. Electrical contacts are applied to the ends, with additional electrical contacts
applied to central portions on surfaces of the width. A voltage is applied across the longitude of the block
(depicted in the x direction) and is labeled Vs . A magnetic field is applied perpendicular to the applied
voltage as shown (depicted in the z direction). Connection across the semiconductor width measures the
induced Hall voltage VH .
The force on a charged particle is described by
F = qe (E + v × B), (15.211)
where v is the charge carrier velocity vector and B is the magnetic field vector. A current I in the sample
of Fig. 15.47 flows in the positive x direction. For p-type material this current is given by
Vs W tVs
I= = = |qe |pW tvh , (15.212)
Rs ρL
680 Basics of Semiconductor Detector Devices Chap. 15

Figure 15.45. The correction factor f2 as a function of


W/s for many rectangular shapes L/W . Also shown is
the correction f2 for a circular sample as a function of the
diameter D/s. Data from Smits [1958].




  
  

 



    


 


 

Figure 15.46. The correction factor f3 as a function of d/s. f3a and
f3b address non-conductive boundaries and f3c and f3d address con-
ductive boundaries. The probes are placed distance d either parallel
or perpendicular to the boundary edge.
Sec. 15.4. Measurements of Semiconductor Detector Properties 681

z B
y
x + EH _
W
EH Ey
_
VH
Ex
+
t
I
L
+ _

Vs
Figure 15.47. Configuration of a Hall effect measurement.

where Rs is the resistance in the longitudinal direction, t is the sample thickness, W is the sample width,
and L is the sample length. Holes accumulate near the negative y surface and produce an electric field. But
a current cannot flow out of the device. The net result is the y forces must be equal and opposite; hence,
the force Fy in the y direction must be zero. Then from Eq. (15.211)

qe Ey = qe vhx Bz or Ey = vhx Bz , (15.213)

where Ey is the Hall field, and the resulting induced voltage VH = Ey W is the Hall voltage. Substitution of
the hole drift speed gives
Bz I IBz
VH = Ey W = W = RH , (15.214)
qe ptW t
where RH is the Hall coefficient and RH = 1/(qe p).
In a similar manner, the Hall coefficient for n-type material is,
1
RH = − . (15.215)
qe n
Therefore, from the measured current and known magnetic field, the hole and electron concentrations are
found as
1 1
p= and n=− . (15.216)
qe RH qe RH
Notice that the resulting positive or negative sign yields the type of majority charge carrier (n or p). The
Hall mobility is determined from
|RH |
μH = , (15.217)
ρ
a useful result, but is not the carrier drift mobility. The actual drift mobility for holes is found by substituting
the resistivity into Eqs. (15.209) and (15.210), namely
μH
μh = , (15.218)
qe p|RH |
682 Basics of Semiconductor Detector Devices Chap. 15

and for electrons


μH
μe = . (15.219)
qe n|RH |
When both holes and electrons are present, the Hall coefficient is represented by [Schroder 1990]
*  2 + 
μe
p−n + (μe B) (p − n)
2
μh
RH =  2 . (15.220)
nμe
qe p+ + (μe B) (p − n)
2 2
μh

Unfortunately, if p ≈ n, the result of Eq. (15.220) can be difficult to interpret.


Overall the Hall measurement can be used to determine the majority charge carrier drift mobility and the
type of majority carrier (n or p). Although the geometry of Fig. 15.47 is perhaps the simplest, it can have
practical difficulties when dealing with thin samples such as epitaxial crystals. Further, errors associated
with the measurement can render RH inaccurate, as outlined in Look [1989]. To address these issues, a
variety of alternative contact geometries have been developed for such cases, as outlined in Look [1989] and
Schroder [1990].

15.4.6 Measurement of the μτ Product


electron-hole substrate
A useful measure of expected performance from a semi-
depletion
region pairs region ohmic
conductor is the mobility-lifetime (or μτ ) product. The
g-ray contact speed of charge carriers can be estimated from the linear
relation v = μE provided that the electric field is below
+
--
the onset of scatter limited saturation speeds. The life-
- +
++
+
- -
-
+ time of a charge carrier is generally defined as the re-
hole electron
blocking motion motion combination time, which can be much longer than the
contact x mean free drift time. The mean free drift time is the av-
0 x1 x’ x2 W erage time period that a charge carrier conducts before
being removed from the process, either by trapping or
Figure 15.48. Electron-hole pairs are excited from a ra-
diation interaction. recombination. Consequently, it is the mean free drift
time that defines the average time between charge car-
rier excitation and its removal from conduction, usually through traps. Hence, it is customary to replace
the lifetime τ with the mean free drift time τ ∗ . For a planar device, the carrier extraction factor can be
described by
vτ ∗ μEτ ∗ μτ ∗ V
= = = . (15.221)
W W W2
In the next section a model is developed for the induced charge in a planar device (see Fig. 15.48) when
trapping is present. The final result Eq. (15.240) is
   
x − W −x
Q(x ) = −qe No e 1 − exp + h 1 − exp , (15.222)
e W h W

where x is the location of the ionizing event. Substitution of Eq. (15.221) into this result gives
$    /
Q V ∗ (x − W )W ∗ −x W
− = 2 μe τe 1 − exp + μh τh 1 − exp . (15.223)
qe No W μe τe∗ V μh τh∗ V
Sec. 15.4. Measurements of Semiconductor Detector Properties 683

From Eq. (15.223) it is observed that the μτ ∗ product yields a measure of the induced charge which has an
effect on the detector energy resolution. The usual method of conducting a μτ ∗ measurement is to irradiate
one of the contacts on a planar detector with an alpha-particle source. The reason for this arrangement is
because the range of alpha-particles is short, confining the excitation of charge carriers in the semiconductor
to a region adjacent to the electrical contact, i.e., x  0. If a planar detector is irradiated from the cathode,
Eq. (15.223) reduces to $  /
Q V ∗ −W 2
− = 2 μe τe 1 − exp . (15.224)
qe No W μe τe∗ V
The μτ ∗ measurement is conducted by observing the relative pulse heights from the detectors at increasing
intervals of voltage. The data is plotted and an interpolative method is used to fit the data to Eq. (15.224).
For high-resistivity materials, W in Eq. (15.224) adequately describes the boundaries of the detector. How-
ever, for detectors requiring depletion to produce an active region, either Eq. (15.59) or Eq. (15.103) is
substituted for W 2 to produce
$  /
Q qe Nb −2 (V − V )
V μe τe∗ 1 − exp
s bi
− = , (15.225)
qe No 2s (Vbi − V ) μe τe∗ V qe Nb

or $  /
Q qe N b ∗ −2s
− ≈ μe τe 1 − exp , (15.226)
qe No 2s μe τe∗ qe Nb
which has the form $  /
Q −1
≈ C1 μe τe∗ 1 − exp , (15.227)
Qo μe τe∗ C1

where the constant C1 = qe Nb /(2s ).


One difficulty with using Eq. (15.226) and Eq. (15.227) is that the value of Q/Q0 appears constant until
the full depletion condition is met, at which point W becomes constant and Eq. (15.224) adequately describes
the measurement.12 The measurement method based on Eq. (15.224) is commonly used to determine the
μτ product, which can then be used in Eq. (15.223) to develop a Q-map for the detector. Measurements
of electron μτ ∗ products are typically easier to conduct than hole μτ ∗ products, mainly because (1) the
mobility of electrons is usually larger than for holes, and (2) τ ∗ is usually larger for electrons than holes.
If the hole μτ ∗ is so small that pulse heights are drastically reduced for anode irradiation, a method
developed by Baciak and He [2003a] may be of practical use. This method involves the accumulation of
pulse height spectra from both cathode and anode irradiation. The centroid of each distribution is chosen to
represent QC  (cathode irradiation) and QA  (anode irradiation). The ratio of charge collected from the
anode QA  and cathode QC   
∗ −W 2
μh τh 1 − exp
QA  μh τh∗ V
=  , (15.228)
QC  ∗
−W 2
μe τe 1 − exp
μe τe∗ V
can be used to extract information about μh τh∗ . This method requires prior knowledge of μe τh so that the
denominator of Eq. (15.228) is known. Hence, the only unknown is μh τh , which is found from Eq. (15.228)

12 The value of τ ∗ often does change with applied voltage, although determining τ ∗ requires knowledge of Nb and μ, and a new
solution for C1 for each voltage increment.
684 Basics of Semiconductor Detector Devices Chap. 15

with iterative methods. There are limitations to the method, mainly because the pulse height distribution
from holes can occupy the lower energy channels and, thereby can be severely contaminated by electronic
noise in the system. Hole pulses lost in the noise and contamination in the pulse height spectrum from noise
can introduce a significant uncertainty in QA .

15.5 Charge Induction


A depiction of a planar semiconductor radiation detector is shown in Fig. 15.48. The detector is separated
into a depletion (or active) region and a substrate region. The substrate region does not contribute to
charge induction but rather acts as a series resistance in the circuit. Hence, charge motion in the depletion
region produces the induced charge under investigation.13 Upon the excitation of electron-holes pairs in the
depletion region, these charges are drifted to their respective contacts, electrons towards the anode and holes
towards the cathode, to produce an induced current. This drifting occurs because of the applied electric
field produced by operating voltage applied across the detector. The charge induction produced by a planar
radiation detector was developed in Chapter 8 (see Eq. (8.44)) and is represented here as
 
x2 − x1
ΔQ = qe N0 , (15.229)
W

where W is the detector width. As also derived in Chapter 8, full charge collection reduces Eq. (15.229) to
Q = qe N0 . Hence, the total charge excited is preserved on the output signal provided that the charge carriers
are collected during the electronic integration time of the detector and circuitry. The other geometrical cases
derived in Chapter 8 also apply to semiconductor detectors, in which the depletion or active region is the
radiation sensitive region.

15.5.1 Charge Induction With Trapping


The ideal cases of charge carrier collection, induced current, induced charge, and the weighting potential
were developed in Chapter 8. However, semiconductors are typically manufactured from crystalline solids
or polycrystalline solids and typically have intrinsic and extrinsic defects. These defects may arise from
vacancies, interstitials, impurities, and complex combinations of defects. Defects may be electrically active,
or may be neutral and serve mainly as scattering centers. Regardless, the presence of crystalline defects
affects the transport of charge carriers, and may serve to trap charge carriers, assist with recombination,
or delay the conduction process so as to effectively remove them from adding to the induced charge of its
corresponding signal.
Four distinguishable trapping and recombination conditions may exist in a semiconductor radiation de-
tector [Dearnaley and Northrop 1966]. These are as follows.

1. Complete carrier extraction in which both electrons and holes are removed from the active region of
the device. Hence, there are no trapping effects.

2. Short-term trapping in which carriers are briefly trapped, but undergo detrapping and are extracted
from the detectors within the shaping time of the pulse. The output pulse may be elongated, and may
suffer from some ballistic deficit, but the charge carriers are collected.

3. Partial recombination of the carriers in which some charge carriers are permanently lost.

13 There are special cases in which there is no actual “depletion region,” but instead only an “active region” defined by the
electric field strength. Under such a condition, the entire semiconductor length can take part in producing the induced charge.
These special cases arise in compensated wide band-gap materials.
Sec. 15.5. Charge Induction 685

4. Long-term trapping in which charge carriers that are trapped are not detrapping during the signal
shaping time. Hence, these trapped charges are also effectively lost. Moreover, detrapping over time
can produce a residual background current.
Consider the design of a common planar semiconductor detector in which electrical contacts are placed
on opposite sides of a planar semiconductor slab. This detector is then irradiated from the side so that the
probability of radiation interactions is constant at all points between the contacts. If a radiation event occurs
at one of the electrodes, the cathode for instance, the pulse is entirely conditional on electron motion. If the
event occurs at the anode, the pulse becomes entirely conditional on hole motion. At other event locations
within the detector, both carriers contribute to the output signal to a greater or lesser degree. If a carrier
collection time is longer than the trapping time, then the effective mobility changes as
τt
μ = μ , (15.230)
τt + τd
where μ is the charge carrier mobility without trapping effects, τt is the mean trapping time and τd is the
mean detrapping time (or average time spent in the trap). Similarly, the charge carrier extraction time t is
reduced to
τt
t = t , (15.231)
τt + τd
where t is the expected collection time in the absence of trapping. If the situation exists in which one
charge carrier follows condition 1 (no trapping), while the other charge carrier follows condition 2 (short-
term trapping and detrapping), the pulse shape is deformed depending on the interaction location of the
radiation absorption.
Building on the results of Sec. 8.6 for a planar detector, the charge induction when trapping occurs can
be derived by first considering the contributions from electrons and holes, namely
   
x2 − x0  x1 − x0 
ΔQ = No −qe − + qe  + , x1 < x0 < x2 , (15.232)
W e W h

No
= (−qe Δxe − (+qe )Δxh ) , (15.233)
W
where No is the number of electron-hole pairs created by a radiation event and x0 is the radiation interaction
location. The corresponding current is
 
dQ −qe No dxe dxh
I= = + , (15.234)
dt W dt dt

in which the signs indicate the unit charge (positive or negative) and direction. Equation (15.234) is rewritten,
after charge carrier speeds and trapping terms are inserted, to yield
dQ −qe No ∗ ∗
I= = ve e−t/τe + vh e−t/τh , (15.235)
dt W
where τe∗ and τh∗ are the mean free drift times for the electrons and holes, respectively, before the charge
carriers are permanently removed from conduction. Integration of Eq. (15.235) yields the induced charge
 te  th 
−qe No −t/τe∗ −t/τh∗ −qe No  ∗ ∗ ∗

Q= ve e dt + vh e dt = ve τe 1 − e−te /τe + vh τh∗ 1 − e−th /τh ,
W 0 0 W
(15.236)
686 Basics of Semiconductor Detector Devices Chap. 15

where the terms te and th are the time intervals required to collect all electrons and holes, respectively, from
their point of origin. The speed is the distance xe,h that a charge carrier travels over time period te,h , so
that Eq. (15.236) can be rewritten as

−qe No xe τe∗ ∗ xh τh∗ ∗


Q= 1 − e−te /τe + 1 − e−th /τh . (15.237)
W te th

The carrier extraction factor is defined as


vτ ∗ xτ ∗ λ∗
≡ = = , (15.238)
W tW W
where λ∗ is the mean free drift length. Equation (15.237) can be rewritten as
   
−xe −xh
Q = −qe No e 1 − exp + h 1 − exp . (15.239)
e W h W

Suppose the detector orientation shown in Fig. 15.48 is chosen for a coordinate system, such that electrons
drift in the positive x direction and holes drift in the negative x direction. For any location x within the
detector, the drift distance for electrons is W − x and the drift distance for holes is simply x . In terms of
x Eq. (15.239) becomes
   
 x − W −x
Q(x ) = −qe No e 1 − exp + h 1 − exp . (15.240)
e W h W

Radiation events occurring at the contacts, at either x = 0 or x = W , reduce Eq. (15.240) to


 
−1
Q = −qe No e 1 − exp , for electron dominated signals, (15.241)
e
 
−1
Q = −qe No h 1 − exp , for hole dominated signals. (15.242)
h

The probability distribution of induced charge is found by multiplying Eq. (15.240) by the interaction
probability distribution function P (x ) where P (x )dx is the probability an interaction creating change Q0
occurs in dx about x . The evaluation of P (x ) generally requires the use of numerical transport theory
if all the various ways photons interact are to be considered. Further, the interaction PDF also generally
depends on the amount of energy deposited as well as the interaction location. The only situation in which
an analytic expression for the interaction probability can be obtained is one in which only the photoelectric
effect is present. This situation is discussed further later in this section.
A special case is one in which P (x ) = 1 for all x , i.e., radiation events occur uniformly throughout the
detector volume. Such a case may be observed for highly penetrating radiation that irradiates the device
from a side between the contacts. In this case
Q(x ) Q(x )
P (x ) → .
Q0 Q0
The pulse height distribution with P (x ) = 1 and with both carrier extraction factors equal is shown in
Fig. 15.49. This Q-map shows that if both charge carrier extraction factors are large (≥ 50), the variance
in the pulse height spectrum is small. This difference is detectable by comparing the largest pulse height
(at x = 0.5) to the smallest pulse height (at x = 0 and x = 1). The Q-map can be interpreted as follows:
Sec. 15.5. Charge Induction 687

Figure 15.49. Q-map for different cases in which e = h . For large values of e and
h , the variance in normalized pulse height is minimal. As  for both charge carriers
decreases, the variance broadens.

Figure 15.50. Q-map for different cases in which e is large (= 50) and h changes.
As h is decreased, the variance broadens.
688 Basics of Semiconductor Detector Devices Chap. 15

a relatively horizontal region in a curve represents the formation of an energy peak in the pulse spectrum,
whereas sloped regions represent the formation of a tail in the pulse height spectrum. The curve in Fig. 15.49
for e = h = 50 is horizontal and indicates that all pulses fall into an energy peak, thereby rendering good
energy resolution. Further, the magnitude of the pulse is nearly 100% of the maximum possible and indicates
that all of the charge carriers are collected. However, the curve for e = h = 0.5 shows a short horizontal
region between x = 0.3 to x = 0.7, an indication that approximately 40% of pulses appear in an energy
peak, while the remaining 60% of pulses appear in a tail. The largest pulse height appears at approximately
63% of the expected value, which indicates severe losses of the charge carriers. Further the tail extends
from 63% of the expected pulse height down to 43% of the expected pulse height. Note that a considerable
horizontal region appears for low values of  < 0.15. However, the expected pulse height is small for these
conditions and indicates that system electronic noise ultimately competes with the radiation signals, thereby
compromising the energy resolution of the detector.
The energy resolution is much worse if e = h , as is usually the case. For example, shown in Fig. 15.50
are several cases in which e is constant at 50 while h is changed. Notably, the signal variance is worse in
all cases than those shown in Fig. 15.49 (except for e = h = 50). For instance, the comparative case with
e = 50 and h = 0.5 indicates the appearance of a small energy peak from events in the region between x = 0
and x = 0.15. Only 15% of interactions accumulate in an energy peak. The remaining signals accumulate in
a tail region extending from approximately 100% of the expected pulse height down to 43% of the expected
pulse height. An example of this result is shown in Fig. 15.51, from which it is clear that the full energy
peak is not Gaussian and most of the pulse height spectrum appears in an elongated tail.
The solution of the variance for Eq. (15.240) can be shown to be [Day et al. 1967; Knoll and McGregor
1993]

3e
2
σQ = qe2 No2 2e + 23e (e−1/e − 1) + (1 − e−2/e ) + 2h + 23h (e−1/h − 1) +
2
3h
(1 − e−2/h )2e h + 22e h (e−1/e − 1) + 2e 2h (e−1/h − 1)
2
(e h )2 −1/e
+2 (e − e−1/h ) − Q2 , (15.243)
 e − h

where  
Q = qe N0 e + 2e (e−1/e − 1) + h + 2h (e−1/h − 1) . (15.244)

The percent fractional standard deviation can be found from


100σQ
σq = , (15.245)
Q

and is plotted as a function of electron and hole extraction factors in Fig. 15.52. Note that the values in
Fig. 15.52 do not depict the energy resolution, typically defined as the FWHM, where the usual definition is
derived from a Gaussian peak, namely

FWHM = 2 2 ln 2σ = 2.355σ. (15.246)

For moderate to severe charge carrier trapping, the peaks in pulse height spectra are usually not Gaussian,
but instead are skewed to the lower energies with a salient tail region and, thus, the use of Eq. (15.246)
is inaccurate. For example, the pulse height distribution for full energy absorption (photoelectric effect),
without Gaussian spreading, is shown in Fig. 15.51 for the case in which e = 50 and h = 0.5. Most of the
Sec. 15.5. Charge Induction 689

Figure 15.51. A comparison of the Q-map for e = 50, h = 0.5 and


the resulting pulse height spectrum with 1000 solution bins divided over
100 channels.

Figure 15.52. The expected percent standard deviation in the observed


induced charge signal as function of e and h . From [Knoll and McGre-
gor 1993].
690 Basics of Semiconductor Detector Devices Chap. 15

distribution appears in a long tail region, with approximately 19% of the events appearing in the full energy
peak. Overall, Eq. (15.240), Eq. (15.243), and Eq. (15.244) serve to illustrate the effect of trapping on the
energy resolution of a planar radiation detector.
Radiation detectors are often irradiated with one side exposed to the source. For instance, the condition
for Eq. (15.240), Eq. (15.243), and Eq. (15.244) is uniform irradiation between the detector contacts, as
with irradiating a semiconductor block from the side between the contacts. Often a detector is irradiated
towards one of the electrical contacts, in which exponential absorption from one contact to the other render
a non-uniform gamma-ray interaction distribution. The resulting pulse height distribution is weighted by
the probability the gamma ray interacts within the detector, thereby changing the result of Eq. (15.240)
and Eq. (15.243), a condition especially true for low-energy gamma rays. If it is assumed that a gamma-ray
deposits all energy for each event in a defined small region (i.e., the photoelectric effect dominates), then
the pulse height distribution for a planar detector can be corrected by multiplying Eq. (15.240) and the
gamma-ray interaction probability density function, namely

Q(x ) Q(x ) μp exp−μp x
P (x ) = , (15.247)
Q0 Q0 1 − exp−μp W
where μp is the photoelectric interaction coefficient which, for low energy photons, is much greater than μC
and μpp for scattering and pair production, respectively. However, the predominant method of gamma-ray
interactions for moderate to high-energy gamma rays is Compton scattering, which further confuses the
evaluation of Q, Q, and σQ2
. Geometries other than planar can be used to improve the energy resolution
by increasing the charge induction influence of one charge carrier over the other, as already described in
Secs. 8.7 and 8.8. Corrections must also be made to the expected value of Q(x) to account for differences
in the induced charge and differences in the gamma-ray absorption probability. Such a calculation is best
accomplished by using transport theory methods to determine location and energy deposited, coupled to the
weighting potential to determine the effect on induced charge, and multiplying the results by Eq. (15.240).
These concepts are further explored in a latter chapter on radiation spectroscopy.

15.5.2 Energy Resolution Improvement Methods and Designs


Because of the severe hole trapping and the degradation in energy resolution, multiple methods have been
developed to improve the spectroscopic performance of CdZnTe detectors [Zhang et al. 2013]. Electronic
corrections such as rise time rejection and rise time correction were introduced to mitigate hole trapping
problems. The usual difficulties accompanied these methods. For instance, rise time rejection helps to elim-
inate undesirable pulses, thereby decreasing the effective volume of the detector and consequently reducing
the efficiency. Rise time correction has also been successfully used, a method that artificially adds “charge”
to the signal as a function of the initial slope of the current and induced charge. More clever methods
used device weighting fields and geometric effects to counter charge loss from hole trapping. These tech-
niques used for Si and Ge detectors altogether eliminated the need for complicated electronics and required
only common preamplifier and amplifier circuits. Finally, there are hybrid detectors that used both clever
weighting potential corrections and rise time corrections to achieve improved energy resolution and detection
efficiency.
Pulse Shape Discrimination and Pulse Rise Time Compensation
Electronic corrections have been used to improve the gamma-ray energy resolution of many different semicon-
ductor detectors, most of them fabricated as planar-style detectors. Jones and Woollam [1975] are credited
with first introducing the idea of improving the results of poor charge collection and trapping effects by
discarding pulses with rise times greater than 100 ns. In so doing, pulses dominated by hole drift were
eliminated, leaving only those pulses that were mainly electron dominated. This technique of discarding
Sec. 15.5. Charge Induction 691

undesirable pulses is referred to as pulse shape discrimination (PSD), and can be used to improve the
spectroscopic performance of detectors in which one type of charge carrier undergoes problematic trapping
[Holzer 1983]. The use of PSD has been reported for CdTe detectors [Richter and Siffert 1992 (shown in
Fig. 15.53); Bargholtz et al. 1999], CdZnTe detectors [Cardoso et al. 2003] and HgI2 detectors [Holzer 1983].
Unfortunately, PSD also reduces the effective volume of the detectors, thereby also reducing the detection
efficiency.

1800

1600
Comparison between selection and
compensation method, normalized
1400 for same initial spectra.

1200

1000

800

600

400

200

0
220 240 260 280 300 320 340 360 380 400 420

Figure 15.53. A comparison of results from a planar 5 mm × 5 mm × 2 mm


CdTe detector. The comparison shows the result for 137 Cs without correction
(light dots), with PSD (blackened spectra), and PRC (black outline). From
Richter and Siffert [1992]; copyright Elsevier (1992), reproduced with permission.

Another electronic method to improve energy resolution was introduced by Matsushita et al. [1981;
1982], and is generally referred to as pulse rise-time compensation (PRC).14 Matsushita et al. applied the
technique to correct for charge losses in neutron damaged Ge or Ge(Li) detectors. The technique can
involve (1) the recognition that the initial slope of the pulse is an indicator of the number of charge pairs
liberated by the radiation event, and (2) the resultant pulse height is a manageable function of the trapping
charge loss. Various methods of accomplishing PRC have been reported, including results by Richter and
Siffert [1992; 1993], Keele et al. [1996], and Auricchio et al. [2005]. Although the method was originally
applied to planar detectors, it was found that PRC could be applied to coaxial and trapezoidal geometries,
although the corrections were complicated by the non-uniform electric fields Matsushita et al. [1981; 1982].
Richter and Siffert [1992] found that the full energy peak shifts linearly with pulse height, thereby allowing an
electronic correction by artificially adding value to a smaller pulse height. The PRC technique gives improved
spectroscopic results while retaining relatively good counting efficiency. Combining PSD and PRC, Ivanov
et al. [1995] report best energy resolution of 1% FWHM for 662-keV gamma rays with a 2 mm × 5 mm ×
5mm detector at room temperature without a decrease in full energy peak efficiency. Although both the PSD
and PRC methods give improved performance, Richter et al. [1993] point out that differences in detector

14 Matsushita et al. [1982] originally named the method the “pulse-height correction” (PHC) technique.
692 Basics of Semiconductor Detector Devices Chap. 15

performance, including problems with space charge limited currents, can diminish the effective use of these
correction methods.

Coaxial and Hemispherical Two-Terminal Devices


In Secs. 8.7 and 8.8 it was seen that the weighting function can be made strongly non-linear by adjusting
the relative sizes of the cathode and anode contacts. The fundamental geometries evaluated were planar,
coaxial and spherical. The problem of using planar designs in the presence of highly trapped charge carriers
was evaluated in Sec. 15.5.1 and the consequences shown in prior sections of this chapter. Lund et al.
[1996] attempted to reduce the effect of hole trapping in CdZnTe detectors by producing coaxial devices;
however, the performance was only marginally improved over that of a planar detectors. Unlike the coaxial
geometry commonly used for HPGe detectors, in which charge carrier trapping for both holes and electrons is
negligible, the non-uniform electric field in a coaxial CdZnTe detector produces non-constant charge carrier
speeds and, consequently, changes in the mean free drift times compromising the performance [McGregor
and Rojeski 1999]. There are relatively few reported results for coaxial compound semiconductor detectors,
mainly because of the difficulty with producing coaxial detectors from soft and brittle semiconductors. A
partial coaxial geometry, literally a wedge segment from a coaxial geometry, was reported by McGregor et
al. [1999] with improved results.
Hemispherical detectors have also been investigated [Malm et al. 1975; Zanio 1977; Alekseeva et al. 1985].
The detectors are semiconductor hemispheres with the rounded surface acting as the cathode with a small
dot anode positioned at the hemisphere focus. The geometric weighting of the device causes most pulses
to originate near the cathode, thereby most pulses are electron dominated and consequently the energy
resolution is improved. The field dependent speed and mean free drift times must also be considered when
predicting the spectroscopic performance. Khusainov [1992] describes the performance of CdTe hemispherical
detectors, slightly chilled with a Peltier cooler, and obtained an energy resolution of 10 keV FWHM at 662
keV. Back in 1992, these CdTe hemispherical detectors were commercially available and in use by the IAEA
for control of SNM. Sensitive volumes reported by Khusainov were, at maximum, only 32 mm3 , while Richter
and Sifferet [1992] report energy resolution averaging about 5% FWHM at 662 keV and show results from a
65 mm3 device. Bale and Szeles [2006] report the results from a commercial “quasi-hemispherical” CdZnTe
detector, fabricated by covering five of the six faces of a semiconductor right cuboid with an electrode that
serves as the cathode, and then placing a small dot anode in the center of the sixth face. A right cuboid
shape is much easier to fabricate than a hemisphere, and the spectroscopic performance is practically the
same, reported to be 20 keV FWHM (3%) for 662 keV gamma rays. The μe τe product limits the practical
radius of the device (see Fig. 15.54), a limitation which is also true for a coaxial detector. While a coaxial
detector volume can be increased without affecting the radius by simply lengthening the device, the same is
not true for a hemisphere. Consequently, the useful volume of a hemispherical device is limited by a radial
dimension that has efficient electron collection.
There is a fundamental problem with almost all two terminal devices designed to enhance the induced
current of one charge carrier over the other; mainly, the weighting potential is the normalized distribution
of the actual operating potential. Although the presence of space charge complicates the analysis by further
altering the voltage and electric field distribution in a detector, for simplicity consider the case without
space charge. Detectors with strongly non-linear weighting potentials also have strongly non-linear operating
potentials, thereby also producing large regions of low electric field. Consequently, the charge carrier speeds
of both electrons and holes are also low in the low electric field region and reduces the μτ products. Detectors
with three or more terminals can be used to counter this problem by decoupling the weighting potential from
the operating potential.
Sec. 15.5. Charge Induction 693

dN
dQ
+V +V

1 2
1 2 0 Qo
low mt high mt dN
dQ
3 -V -V 4

4
3
0 Qo

Figure 15.54. Expected pulse height spectra from a hemispherical de-


tector with severe hole trapping for four cases: (1) positive focus with
low μe τe , (2) positive focus with high μe τe , (3) negative focus with low
μe τe , and (4) negative focus with high μe τe . After Malm et al. [1975].

Weighting Field Optimization


Another method to improve spectroscopic resolution employs clever electrode designs to force the appearance
of strongly non-linear weighting potentials [Zhang et al. 2013]. These electrode designs are used to enhance
the importance of charge induction of one charge carrier type (usually electrons) while reducing or negating
the influence of the other charge carrier (usually holes). Quite often these detectors are referred to as single
carrier detectors. There are many such designs and a few important types are briefly described here.
A common method used to solve the detector weighting potential is to employ Laplace’s equation

∇2 φ = 0, (15.248)

where φ is the electrical potential. As explained in Section 8.6, space charge does not affect the weighting
potential and, hence, Laplace’s equation is used instead of Poisson’s equation. Equation (15.248) is solved
with the boundary conditions that the output conductive contact is normalized to one volt and all other
contacts are grounded at 0 volts. This computational method is described and used by Shockley [1938].15
Radiation spectrometers with optimized weighting fields to improve performance are often designed
with the methods introduced in Chapter 8. Although simple designs using planar, coaxial, and spherical
geometries are easily calculated with analytical methods, complex geometries and electrode patterns require
numerical methods to analyze the weighting field and weighting potential. There are available many finite-
difference software programs designed to analyze the electric fields and voltage potentials within a dielectric
material.
Co-Planar Grid Luke [1994, 1995] introduced a contact geometry referred to as the coplanar grid detector.
The method mimics the Frisch grid ion chamber. The detector is generally planar in form, with a planar
cathode contact on the lower surface and a series of parallel contact strips on the upper surface. It has

15 Themethod is derived from Green’s theorem, although over the years it has been named Ramo’s theorem or the Shockley-Ramo
theorem. The core solution is derived from either Green’s theorem or the reciprocal Green’s theorem.
694 Basics of Semiconductor Detector Devices Chap. 15

boundary electrode

anode 1

anode 2

Figure 15.55. Simple coplanar grid design (on left) and a balanced coplanar
grid design (on right).

no actual drift region as with the Frisch grid ion chamber, but instead has a virtual drift region defined
by the strip widths and pitch as shown in Fig. 15.55. In the original work, alternating contact strips were
connected to two different preamplifiers, labeled in the present case as high and low preamplifiers. The high
contacts operate as collecting anodes and the low contacts act as secondary non-collecting anodes with a
lower positive voltage than the collecting anodes. Both contacts are biased positively with respect to the
planar back cathode.
The signal from the low preamplifier is subtracted from the signal of the high preamplifier, thereby
producing a virtual Frisch grid effect. As electron charge carriers move toward the anodes, they induce
current to flow on all anodes, both collecting and non-collecting. At distances relatively far from the anodes,
these induced currents are practically identical, hence, the net output result is zero. The same is true for
hole charge carriers moving in the opposite direction. However, as charge carriers reach the strip electrodes,
the higher bias applied through the high preamplifier causes electrons to turn into the collecting electrodes,
producing a positive current flow on the high preamplifier and negative current flow on the low preamplifier.
As electrons are completely collected, the net subtracted result between both outputs is the appearance of
full charge collection on the combined output. Because holes move the opposite direction towards the planar
back electrode (cathode), their net contribution is practically zero, thereby negating the deleterious effect
of trapping. The biasing scheme and resultant induced signal are depicted in Fig. 15.56, and the resulting
weighting potential is shown in Fig. 15.57. Although the improvement was dramatic and an important
innovation for room temperature radiation spectroscopy, effects from electron trapping and weighting field
imbalances between the anode strips caused broadening of energy peaks. The resulting full energy peaks
typically had low and high energy tails, producing a flared appearance to the base of the energy peak, and
thus limited the improvement in energy resolution.
He et al. [1998] and Sturm et al. [2004] corrected the weighting field imbalance by optimizing the coplanar
strip design, which included two balancing strips around the coplanar strips with an additional boundary
electrode around the detector perimeter as shown in Fig. 15.55. In doing so, He et al. [1998] dramatically
improved the performance of the coplanar grid detector. The flared base of the full energy peak was prac-
tically eliminated, and with charge compensation through electronic methods, energy resolution below 2%
FWHM at 662 keV was usually realized. This balanced configuration, in various forms, is now a standard
design feature for commercial coplanar grid CdZnTe detectors.
Sec. 15.5. Charge Induction 695

Small Pixel Detectors Detectors with pixels have been fabricated from a variety of semiconductors, includ-
ing Ge, Si, GaAs, and CdZnTe, for the purposed of two-dimensional imaging of radiation. Ultra-small pixels
on CdZnTe detectors were initially introduced by Doty et al. [1992]; however, it was Barrett et al. [1995] who
identified what is now commonly referred to as the small pixel effect by analyzing the results from pixelated
CdZnTe detectors. The basic design is essentially another two-terminal device, but there is instead an array
of small pixel anodes on one surface and a single planar cathode contact on an opposing surface as shown
in Fig. 15.58. Barrett et al. [1995] correctly point out that the weighting potential is strongly non-linear
for each pixel, giving stronger influence to charge carriers moving near the anode pixels. As charge carriers,
electrons for instance, approach any particular pixel, the induced charge accumulates almost entirely on a
single pixel. Hence, connecting separate outputs to each pixel allows one to determine the charge location
while benefiting from improved charge collection. For pixel size  ×  and detector thickness L, the total
induced charge for electron-hole pairs excited at location z = 0.2L near a pixel is plotted as a function of
ratio /L in Fig. 15.59. From this figure it becomes clear that the single carrier effect becomes stronger as
the /L ratio diminishes.
If the same operating potential is applied to all pixels, the overall effect is to have a near constant electric
field across the detector thickness, thereby negating the non-uniform electric field effects observed with
cylindrical, trapezoidal, and hemispherical detectors. The simple pixel design, however, suffers from charge
sharing and charge loss problems. Charge sharing is caused by electrons produced by a single initial event
are collected by two or more electrodes, and causes pulse height reduction on all electrodes involved. Charge
loss is caused by trapping of slow moving electrons in the low field region between pixels, ultimately reducing
the pulse height.
The small pixel effect can be enhanced by adding a third electrode around the pixels (see Fig. 15.58),
which performs as a non-collecting steering electrode much like that in the co-planar grid [He 1995]. Under
such a condition, the pixels can be biased positive with respect to the steering grid, while the steering grid

(a) Q

C
Y

X B

Q0

(b)
qA
Induced
Charge (qA - qB)
qB

0
Distance

Figure 15.56. Shown are (a) the basic structure of a Figure 15.57. Weighting potential distribution for the set
coplanar grid detector, (b) induced charge on the electrodes of collecting grid electrodes in the coplanar grid configura-
A (qA ) and electrodes B (qB ) and the resultant difference tion. Reproduced from P.N. Luke, Appl. Phys. Lett., 65,
signal. After Luke [1995]. 2884, (1994), with the permission of AIP publishing.
696 Basics of Semiconductor Detector Devices Chap. 15

Figure 15.58. Simple pixel detector design (left), a pixel detector design with a steering
grid (middle), and a hybrid pixel-strip design (right).
No Trapping Case Total
1

holes
0.8
Charge Q/Q0

0.6
L
holes z/L = 0.2
electrons
0.4

0.2
electrons

0
0 1 2 3 4
Pixel Width (e/L)

Figure 15.59. Total collected charge for holes and electrons excited at depth
Z = 0.2L as a function of pixel size. After Barrett et al. [1995].

is biased positive with respect to the cathode. Usually the pixels are just a few volts higher in positive bias
than the grid, enough to efficiently collect electrons while minimizing leakage current between the anodes
and grid. Hence, the steering grid functions as a non-collecting electrode which (1) assists with electrically
steering electrons into a collecting pixel and (2) reduces the leakage current impact on the anode outputs
[He et al. 1999]. Energy resolution was further enhanced by applying electronic correction methods to the
pixel/grid structure. Because a lateral electric field is applied between the grid and pixels, the steering grid
helps reduce the problem with charge losses observed in simple grid designs.
Another pixelated electrode configuration, a hybrid between a pixel detector and a strip detector, was
studied by Mayer et al. [1999] and Montemont et al. [2007]. Each strip electrode has an embedded row of
pixels, in which the strip acts as the non-collecting electrode. The design attempts to produce a simple
scheme for two-dimensional radiation imaging, thereby greatly reducing the number of electronics readout
points from a basic pixel detector, while retaining the advantage of the small pixel effect. The strips each have
a separate readout and operate as steering grids, while the rows of pixels are interconnected, each row having
a separate readout (see Fig. 15.58). Readout information from the x-y grid yields position information, while
the small pixel effect improves gamma-ray energy resolution.
Sec. 15.5. Charge Induction 697

Trapezoid
Trapezoid
Width
Height

Center Slice
Through Width Cathode
End

Anode
End

Frisch Grid
Strip Frisch Grid
Strip

Figure 15.60. A 3-D depiction of a trapezoid frus- Figure 15.61. The weighting potential of a trape-
tum semiconductor Frisch grid detector. Also shown zoid frustum geometrically weighted CdZnTe Frisch
is a plane sliced through the middle of the device. grid detector, sliced through the center of the de-
From McGregor et al. [2001]. tector as shown to the left. After McGregor et al.
[1999a].

Frisch Style Constructions McGregor et al. [1997; 1998] introduced the parallel strip and geometrically
weighted parallel strip CdZnTe detector designs in 1997. The simplistic design required only one preamplifier
output, and was designed to mimic the operation of a Frisch grid ion chamber. The detector consisted of a
CdZnTe bar, nominally 2-3 mm thick, with surface areas of 5 mm × 5 mm or 10 mm × 10 mm. Parallel
edges of the planar device had electrical contacts applied. On opposite surfaces, centering approximately 1
to 2 mm from one edge contact, gate contacts were applied through physical vapor deposition. One edge
contact was biased negatively, the parallel gate contacts were grounded, and the output anode edge contact
was biased positively through a commercial preamplifier. Room temperature energy resolution of 41 keV
FWHM for 662-keV gamma rays was reported for a 1 cm × 1 cm × 2 mm device. The device worked to
demonstrate the concept, and was later improved by using a trapezoidal frustum shape. The small end of
the frustrum operated as the output anode, the large bottom of the frustum operated as the cathode, that
the gate electrodes were centered at 1.5 mm from the anode (see Fig. 15.60 and Fig. 15.61). As explained
in the literature [McGregor et al. 1999a; McGregor and Rojeski 1999b, 2001], more gamma-ray interactions
occur in the drift region near the base, thereby causing the majority of pulses to be electron dominated. The
multiple-electrode design provides the benefits of both a non-linear weighting potential and also, through
appropriate application of voltages to the anode and grid, a nearly uniform electric field through the detector.
Room temperature energy resolution of 17.76 keV FWHM for 662-keV gamma rays was reported for a 1 cm3
device. Initially there were some issues with leakage current between the grid and anode. Theory shows that
the grid need not be in direct contact with the semiconductor; hence, surface leakage current was practically
eliminated by applying a thin Al2 O3 layer atop the semiconductor sides, followed by the application of the
698 Basics of Semiconductor Detector Devices Chap. 15

grid strips. Although the trapezoid Frisch grid detectors worked well,16 the detector cutting, shaping, and
polishing proved challenging and difficult to fabricate.
McGregor and Rojeski [2001] (and McGregor [2004]) intro-
duced another simple device, commonly referred to as either a
Anode Anode Frisch collar detector or Frisch ring detector, depending on the
Insulating
length of the gate contact (see Fig. 15.62). The detector is de-
Layer signed as an elongated semiconductor bar with contacts at each
end. The bar is wrapped in an insulating coating followed by
Conductive a conductive wrapper or sleeve. The insulating layer eliminates
Semiconductor Foil Semiconductor
leakage current between the Frisch ring/Frisch collar and the
collection electrode. Much like the strip grid designs, the Frisch
ring design produces both a non-linear weighting potential and,
with the proper application of potentials to the grid ring and an-
Cathode
ode, a nearly uniform electric field throughout the detector (see
Fig. 15.63). However, the Frisch collar design is simpler to man-
Figure 15.62. Cross section depictions of a ufacture than the trapezoid or Frisch ring designs, and generally
(left) Frisch collar and (right) Frisch ring semi- produces better energy resolution, despite being a two-terminal
conductor detector. device. The conductive wrapper or sleeve is grounded and the
remaining anode contact is positively biased.
The first such detector was reported by McNeil et al. [2004] whose detector had dimensions of 3 mm × 3
mm (area) × 6 mm (length). Electroless gold contacts were applied to the 3 mm × 3 mm ends and Teflon
tape was wrapped around the bar as the insulator. Afterwards, thin Cu foil was used as the conductive
wrapper. Using a commercial charge sensitive preamplifier, the detector delivered room temperature energy
resolution of 15.3 keV FWHM (2.31%) for 662 keV gamma rays. Kargar et al. [2006; 2009] and Harrison et al.
[2009] worked to optimize the design and performance of the Frisch collar detector, eventually achieving room
temperature energy resolution of 5.9 keV FWHM (0.89%) for 662 keV gamma rays [Ugorowski et al. 2011].
It was discovered that performance improved as the dielectric constant of the insulating layer decreased,
and Teflon tape, with a dielectric constant of only 2.1, was an obvious choice and yielded superior results
over alternative insulators, including Al2 O3 and SiO2 . The Frisch collar design has also been successfully
applied to HgI2 detectors [Ariesanti et al. 2010, 2011; Kargar et al. 2011a, 2011b], and a 2.1 mm × 2.1 mm ×
4.1 mm device yielded room temperature energy resolution of 11.9 keV FWHM (1.8%) for 662 keV gamma
rays. A considerable advantage of the Frisch collar design is the simple construction from a common planar
bar of semiconductor material and low cost materials, thereby eliminating the need for electrode patterning
altogether. These detectors can be arranged in an array for imaging purposes [McGregor 2004; Cui et al.
2007, 2008; Ugorowski et al. 2011]. The robustness of the Frisch collar design has been verified by other
research groups [Kim et al. 2015; Jeong et al. 2015; Bolotnikov et al. 2012].

Drift Style Detectors The semiconductor drift chamber (SDC), originally designed for large area Si detec-
tors [Gatti and Rehak 1984; Rehak et al. 1985, 1986], has been adapted to compound semiconductors as a
means of countering the effects of charge carrier trapping. The original intent of the SDC was to increase
the active area of a semiconductor detector while reducing capacitive noise. The basic design uses a series
of microstrip electrodes, either in a linear array or a series of concentric circles (bull’s eye) on opposing sides
of a semiconductor block [Rehak et al. 1985; Bertuccio et al. 1992]. At least one of the electrodes serves as
an anode, while the remaining electrodes serve as guiding electrodes. These guiding electrodes are biased

16 Atthe time, the trapezoid parallel strip detectors set the room temperature resolution record for CdZnTe, but was surpassed
by other technologies within only a few years.
Sec. 15.5. Charge Induction 699

Figure 15.63. Comparison of weighting potentials from a (left) planar device, (middle) Frisch ring device, and (right)
Frisch collar device. Each detector is modeled as a 5 mm × 5 mm × 10 mm CdZnTe detector. The insulating material
is 100-micron thick Teflon.

V-- ................. V- ................. V--


Guiding electrodes (cathodes)
-+
Anode
-+
-+
Guiding electrodes Guiding electrodes
-+
V-- .................. V+ .................. V--
Figure 15.64. Side view depicting the operation of a semiconductor
drift chamber.

so as to drift electrons to the anode, typically a bias scheme with sequentially increasing positive electrodes
towards the anode or sequentially decreasing negative electrodes toward the anode (see Fig. 15.64).
Immediately one can observe that the electrode geometry has much in common with the coplanar, pixel,
and Frisch style detectors, in which most of the induced charge accumulates on the anode as electrons are
transported in the region nearest the anode [Patt et al. 1996]. Consequently, the SDC can be operated
as a single carrier device for materials with hole trapping problems. Patt et al. [1996], van Pamelen and
Budtz-Jørgensen [1998], and Kuvvetli et al. [2001, 2005] describe HgI2 and CdZnTe SDCs with linear array
strips while Owens et al. [2007] reports on a CdZnTe SDC with a concentric ring pattern. These detector
configurations show improved performance over simple planar detectors. Van Pamelen reports 6.89 keV
FWHM (1.1%) for 662-keV gamma rays on a small (1.5 mm thick) CdZnTe detector and Patt et al. [1996]
report 6.62 keV FWHM (1%) for 662-keV gamma rays on a small 6 mm × 6 mm area × 2 mm thick
HgI2 detector. An alternative drift style detector was reported by Butler [1997], composed of a single pixel
surrounded by a drift/focusing electrode. A planar cathode was applied upon the opposing surface. The
detector was operated by applying equal negative voltage to the focusing electrode and cathode with respect
to the anode17 [Apotovsky et al. 1997]. A best energy resolution of 3.67 keV (0.72%) at 511 keV was reported
for a 3 mm × 3 mm × 3 mm cube of CdZnTe.
Hybrid Improvements
Resolution improvement has also been realized by combining multiple effects, particularly, PRC methods
with single carrier detector designs. The use of PRC methods helps to offset energy degradation from electron

17 Named “Spectrum Plus” detectors, these devices were commercially available for a short time during the late 1990s.
700 Basics of Semiconductor Detector Devices Chap. 15

trapping. He et al. [1998] introduced hybrid solutions with balanced co-planar grid detector geometries to
achieve energy resolutions on the order of 1% FWHM at 662 keV. The combination of the small pixel effect
with PRC methods has also been explored by He et al. [1999] who reported a high energy resolution of less
than 1.5%. An added benefit of the hybrid pixelated detector is the ability to determine the interaction
location within the bulk of the semiconductor detector as a function of x, y and z. Consequently, using
Compton scattering deconvolution methods, the actual direction of a gamma-ray source (or sources) can
be determined in a relatively short time [Wahl et al. 2015]. These hybrid methods have been successfully
applied to different compound semiconductors, including CdZnTe [Wahl et al. 2015], HgI2 [Baciak and He
2003a, 2003b], and TlBr [Hitomi et al. 2008].

PROBLEMS

1. Determine the following:


(a) kT at 300 K
(b) kT /qe at 300 K
(c) The band-gap energy of Si and Ge at 300 K

2. Calculate the electron and hole concentrations, the material resistivity, and the Fermi energy level for
Si doped with p = 5 × 1015 cm−3 with background dopants n = 3 × 1015 cm−3 .

3. An Si pn junction diode has NA = 8 × 1017 cm−3 and ND = 5 × 1015 cm−3 , with τp = 10−7 s and
τn = 10−6 s, with the device area of A = 25 mm−2 . (a) Determine the theoretical saturation current at
300 K. (b) Calculate the forward and reverse currents at ±0.7 V.

4. A Si pn junction diode has NA = 1017 cm−3 and ND = 1015 cm−3 . Calculate the value of Vbi for T =
100 K, 200 K, 250 K, 300 K, 350 K, 400 K, and 500 K. Determine both W and Emax at 300 K.

5. It is the goal in making a semiconductor detector to create the largest possible depletion width. Explain
how this goal is best realized by using the purest semiconductor material available.

6. Given a 600-micron thick Si semiconductor pνn diode with p = 1016 cm−3 , ν = 1012 cm−3 , and n = 1016
cm−3 , find the depletion width when reverse bias of 100 volts is applied. What is the depletion width
if the reverse bias is increased 300 volts?

7. You have a Si pνn junction device that is 150 microns wide with ν = 1013 cm− 3 . Determine the punch
through voltage. Determine the breakdown voltage.

8. Describe quantitatively how the magnitude of the reverse bias applied to a p-n junction affects (a) the
device capacitance, (b) the width of the depletion layer, and (c) the maximum electric field.

9. Given a 1.2-micron sample of CdS with a shallow trap density of 1015 cm−3 , what is the expected value
of VT F L ?

10. A young engineer under your direction comes up with the idea of stacking two identical semiconductor
detectors in series and applying the bias across both detectors. What is the expected output and the
consequence of this device circuit?
References 701

11. An n-type Si photoconductor bar (dimensions W1 = 0.1 mm, W2 = 0.01 mm, L = 2 mm) is uniformly
illuminated for a period of time τn , where n = 1014 cm−3 , τ = 1 μs, and T = 300 K. If the initial
illumination produces a generation carrier density of G(0) = G0 = 1016 cm−3 , and turned off at t = 0,
what is the time dependent value of Δn? At 5 volts bias, what is the measured current as a function of
time?

12. Explain how and why the energy resolution of a surface barrier detector changes as the surface area of
the detector is increased.

13. Calculate and plot the Q-map for the case in which the ratio of e /h is constant at 10, with e values
of 50, 25, 0.5, 2.5, 0.5 and 0.05. Comment on the expected pulse height distributions. How would you
design a planar detector to ensure good energy resolution?

14. For an ideal p-type MOS structure (NA = 5 × 1015 cm−3 ) with an oxide thickness of 30 nm, determine
the threshold voltage VT for strong inversion. Note that κ = 3.9 for SiO2 and 11.9 for Si.

15. Derive the result of Eq. (15.244).

16. Derive the result of Eq. (15.243).

17. Starting with the material resistivity ρ very high, such as with a semi-insulating material, derive the
result of Eq. (15.189). Explain the consequence of this finding.

18. You have introduced an n-type dopant into a Si surface, and the backplane has a conductive layer. The
doping depth is 1.5 microns and the feature size is 1 cm L × 0.5 cm W. Using a four-point probe with
spacing of 1.5 mm between the probes, you measure 5 μA at 3 volts. What is the resistivity of the
doped region?

19. Derive Eq. (15.247).

20. Given a CdZnTe hemispherical detector with anode r1 = 1 mm and cathode r2 = 6 mm, calculate the
weighting potential of the device. What fraction of the induced charge is from electrons if a gamma-ray
is completely absorbed at r = 2 mm, 3 mm, 4 mm, and 5 mm? Suppose that trapping is present with
τe = 10−6 s, if τe τh , explain why these outcomes are important.

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and GaP,” Appl. Phys. Lett., 8, 111–113, (1966a). 2474, (2013).
Chapter 16

Semiconductor Detectors

I have lately met with an extraordinary case ... which is in direct contrast with
the influence of heat upon metallic bodies ... On applying a lamp ... the
conducting power rose rapidly with the heat ... On removing the
lamp and allowing the heat to fall, the effects were reversed.
Michael Faraday

16.1 Introduction
Semiconducting behavior was first discovered by Faraday in 1833 when he observed that current flow through
AgS increased with temperature,1 the opposite effect observed with conductive metals. We now know this
effect to be a consequence of increased free charge carrier densities in the conduction and valence bands as
temperature is increased. Decades later, Braun [1874] observed rectifying behavior from a point contact on
a PbS crystal, in which current would flow in only one direction, but not the other, when positive voltage
was applied, alternately, to the sample. This fundamental semiconductor physical property would be used
nearly a century later as a building block for semiconductor diode and transistor designs.
Soon after the development of the gas-filled detector by Hans Geiger and Ernest Rutherford, some interest
was placed in discovering a solid-state material for radiation detection. The concept, correctly, was to increase
the radiation detection efficiency by substituting the gas medium with a solid-state medium. Perhaps the
earliest recording of such an effort was a study performed by Röntgen and Joffé [1913] on various solids
exposed to high levels of x radiation, followed by another study in 1921. Additional work by Schiller [1926]
and Jaffé [1932] revealed conduction through dielectric crystals upon the application of high voltages and
high irradiation fields. Yet, none of these works resulted in the practical application of solid state conduction
counters.
The first semiconductor-based radiation detector was reported by Stetter in 1941, in which several materi-
als were exposed to α-particles, β-particles, and protons. As with earlier works, most of those materials were
insulators (alkali halides, sulphur, cerrusite, fluorite) resulting in no observed effect; however, Stetter also
reported the observation of electrical current from a diamond sample exposed to ionizing radiation. Several
years later, Van Heerden [1945; 1950a; 1950b] published his work on AgCl crystals, “The Crystal Counter”,

1 Published account is in his book Experimental Researches in Electricity [1839].

705
706 Semiconductor Detectors Chap. 16

Table 16.1. Chronological initial exploration dates as radiation detectors for selected semiconductors.

Common
Semiconductor Year Reference
Abbreviation

Diamond diamond (C) 1941 Stetter


1947 Wooldridge, Ahearn & Burton
1948 Curtiss and Brown; Jentschke
Silver Chloride AgCl 1945 Van Heerden
1947 Hofstadter, Milton, Ridgway
Cadmium Sulphide CdS 1947 Frerichs
1948 Kallman and Warminsky
Thallium Bromide TlBr 1947 Hofstadter
Thallium Iodide TlI 1947 Hofstadter
Zinc Sulfide ZnS 1948 Ahearn
Argon (solid) Ar 1948 Hutchinson
Silver Bromide AgBr 1949 Yamakawa
Mercury Sulfide HgS 1949 Ahearn
Sulphur† S 1949 Georgesco
Germanium Ge 1949 McKay
Sodium Iodide NaI 1950 Witt
Silicon Si 1958 Davis
Gallium Arsenide GaAs 1960 Harding
Cadmium Telluride CdTe 1967 Autagawa, Zanio and Mayer
Mercuric Iodide HgI2 1971 Willig
Lead Iodide PbI2 1971 Roth and Willig
Cadmium Zinc1−x Telluridex CZT 1992 Doty et al.
† Stetter [1941] also studied sulphur, but with negative results.

widely accepted as the first reported semiconductor detector.2 Upon the publication of Van Heerden’s work,
numerous semiconductor materials were subsequently investigated, and the investigators along with their
introductory years are tabulated in Table 16.1.
Up until 1960, semiconductor detectors, then called “crystal counters”, were considered mostly a novelty
for radiation detection and were not commercially produced. The main reason, as expressed by Price [1958,
1964], was that semiconductors were of “very little use because of the preponderance of advantages of the
scintillation detectors”.3 A significant disadvantage of semiconductors at the time was the high level of
background impurities and crystal defects. Under reverse bias, the impurities could become ionized, as
explained in Sec. 15.3.5, and trapping of electrons or holes in the defect states would reduce the induced
current. In both cases, space charge would be created which tends to counter the applied voltage and reduce
both the electric field and the depletion region width. However, in 1960 while working for the General Electric
Co. (GE), Erik M. Pell [1960a, 1960b] developed a method of introducing a compensating Li ion into Si that
countered the effect of p-type dopants. The method included the application of Li material to a heated bulk
Si sample and driving Li ions deep into the semiconductor with a strong electric field, a method known as “Li
drifting”. The technique was successfully applied to Si [Pell 1960b; Elliot 1961; Blankenship and Borkowski
1962] and Ge crystals [Freck and Wakefield 1962; Tavendale 1963, 1966; Goulding and Hansen 1964; Goulding
1965, 1966], and allowed relatively thick depletion layers to be formed. It was this fundamental improvement

2 Although Stetter reported his observation years earlier, the work went largely unnoticed. Consequently, Van Heerden has
often been quoted as the originator of the first semiconductor detector. Jeschke attempts to correct the record in his 1948
letter to the editor.
3 Price retracted this opinion in his 1964 book.
Sec. 16.2. General Semiconductor Properties 707

that allowed semiconductors to become important radiation detectors, and Ge(Li) and Si(Li) detectors4
came into common use as high resolution gamma-ray and x-ray detectors.
A drawback to all Ge(Li) detectors was that they required constant cryogenic cooling. If the crystal were
to rise in temperature, the Li ions would diffuse away from their compensation locations and the crystal
would be ruined. Ge crystals could be re-drifted once, maybe twice, but almost always resulted in lower
energy resolution performance. Si(Li) detectors did not suffer the same Li ion diffusion consequence at room
temperature, but both Ge(Li) and Si(Li) detectors perform best when operated at or near the temperature
of liquid nitrogen (LN2).
A solution to the nuisance of cryogenic cooling for Ge(Li) was explored by two research teams, one team
led by Robert Hall at GE and the other team led by William Hansen at the Lawrence Berkeley Laboratory
(LBL) [Haller 1996]. The concept was to apply the zone refinement purification technique developed by
William Pfann [1966], thereby purifying Ge to such a level that it was practically devoid of impurities and,
hence, no longer in need of Li compensation. Both teams succeeded in the mission and produced virtually
intrinsic high-purity Ge crystals, or HPGe crystals. Detectors fabricated from this material no longer required
constant cooling, but still required cryogenic cooling during operation in order to reduce leakage currents.
By the early 1970s, zone refined HPGe, high purity Si, and Si(Li) detectors became standard instruments
for radiation spectroscopy.
Yet, the required cryogenic cooling during operation remains inconvenient. There are solutions, mainly,
low vibration refrigerators or small handheld dewars can be attached to HPGe detectors. Wide band-gap
semiconductors, such as GaAs, CdTe, HgI2 , and CdZnTe (or CZT), that can operate at room tempera-
ture (RT) without cryogenic cooling have been investigated as alternative semiconductors for gamma-ray
spectroscopy. Perhaps to date the most successful of these RT candidates is CZT, mainly because of the
introduction of “single carrier” detector designs by Eskin et al. [1995], Luke [1995], McGregor and Ro-
jeski [1998, 1999], and McGregor [2004]. Included in the present chapter are descriptions of properties for
semiconductors important for radiation detection. Descriptions of semiconductor detectors that are either
commercially available, or at least show great promise for various radiation measurement applications, are
also described in the present chapter.

16.2 General Semiconductor Properties


Desired properties of a semiconductor radiation detector vary with its application. For instance, materials
with low atomic numbers are best used for detection of β particles and electrons while materials with high
atomic numbers are best for detection of x rays and gamma rays. High energy resolution generally requires
a low ionization energy, best accomplished by choosing semiconductors with relatively narrow band gaps.
A small ionization energy causes increased numbers of excited charge carriers, thereby improving statistics
and enhancing spectroscopic energy resolution. However, semiconductor detectors fashioned from narrow
band-gap materials generally require cryogenic cooling during operation. A wide band-gap energy (> 1.5
eV) and high resistivity allow room temperature operation that otherwise would require cryogenic cooling
to reduce electronic noise, but at the price of reduced spectroscopic energy resolution. Other properties
sought for gamma-ray detectors include high atomic density, long charge carrier lifetime, high resistivity,
and high electron and hole mobilities. High atomic density and high Z components increase the γ-ray
interaction probability (see Fig. 16.1). Long charge carrier lifetimes and high charge carrier mobilities
increase the charge collection efficiency and produce better spectroscopic results. Unfortunately, no existing
semiconductor actually has all of these characteristics; hence the investigator should select a semiconductor

4 Pronounced “jelly” and “silly” detectors.


708 Semiconductor Detectors Chap. 16

Table 16.2. Common semiconductors used as radiation detectors and their properties at 300K.
Atomic Ionization Dielectric
Density Fano
Semiconductor Number Structure Energy Constant
(g cm−3 ) Factor
(Z) (eV/e-h pair) (s /0 )

C (diamond) 6 3.5 FCC/Dia. 0.38 13 5.7


Si 14 2.33 FCC/Dia 0.115 3.61 11.9
Ge 32 5.33 FCC/Dia 0.13 2.98 16
CdSe 48/34 5.8 Hex/W 5.5 10.6
CdTe 48/52 5.86 FCC/ZB 0.11 4.43 10.36
Cd0.85 Zn0.15 Te (CZT) 48/30/52 6.0 FCC/ZB 0.089 5.0 10.63
GaAs 31/33 5.32 FCC/ZB 0.1 4.2 13.1
GaSe 31/34 5.03 Hex 4.5 8
HgI2 80/53 6.4 Tetragonal 0.19 4.42 8.8
InP 49/15 4.79 FCC/ZB 4.2 12.5
PbI2 82/53 6.2 Hex 0.19 4.9 4.3
SiC(3C) 14/6 3.21 3C/ZB 5.5 9.72
SiC (4H)   Hex/4H/W 7.8 9.66
SiC (6H)   Hex/6H/W 0.09 6.9 9.66
TlBr 81/35 7.56 BCC 6.5 29.8

Table 16.3. Common semiconductors used as radiation detectors and their properties at 300K.
Band Intrinsic Electron Hole Electron Hole
Semiconductor Gap Resistivity Mobility Mobility Lifetime Lifetime
(eV) (Ω-cm) (cm2 /V·s) (cm2 /V·s) (sec.) (sec.)

C (diamond) 5.47 (I) > 1012 2400 2100 < 10−9 < 10−9
Si 1.12 (I) > 5 × 104 1500 450 > 10−3 > 10−3
Ge (77 K) 0.72 (I) > 1018 36000 42000 > 10−3 > 10−3
Ge (300 K) 0.68 (I) ≈ 50 3900 1900 > 10−3 > 10−3
CdSe 1.73 (D) 108 720 75 10−6 10−6
CdTe 1.52 (D) 109 1050 100 3 × 10−6 2 × 10−6
CZT 1.60 (D) 1011 1350 120 10−6 5 × 10−8
GaAs 1.42 (D) ≈108 8500 400 10−9 − 10−8 10−9 − 10−8
GaSe 2.1 (D) 60 215 2 × 10−6 5 × 10−6
HgI2 2.13 (D) 1013 100 4 > 10−6 > 10−6
InP 1.35 (D) 107 4600 150 1.5 × 10−9 < ×10−7
PbI2 2.3 (D) 1012 8 2 10−6
SiC (3C) 2.36 (I) 150 800 320
SiC (4H) 3.23 (I) > 1015 900 120 4 × 10−7 6.7 × 10−7
SiC (6H) 3.05 (I) 400 90
TlBr 2.68 (I) 1012 6-25 1.5-6.2 ∼ 2.5 × 10−6 ∼ 4.3 × 10−6

detector best suited for the desired application. The basic properties of several semiconductors used for
semiconductor detectors are listed in Tables 16.2, 16.3, and 16.4.

16.2.1 Atomic Numbers and Mass Density


The choice of detector material depends on the type of radiation to be detected. As discussed in Sec. 7.2.1
and Sec. 7.2.2, the backscatter coefficient for charged particles (both electrons and alpha particles) increases
with the atomic number of the absorber. Likewise the absorption coefficient for photons (see Sec. 4.4) also
increases with the atomic number of the absorber. Hence, it is generally better to fabricate charged particle
detectors from low Z materials, such as Si. By contrast, high Z materials are preferred for gamma-ray
Sec. 16.2. General Semiconductor Properties 709

Table 16.4. Common semiconductors used as radiation detectors and their properties at 300K.
Semiconductor NC (cm−3 ) NV (cm−3 ) m∗t m∗l m∗o m∗lh m∗hh

C (Diamond) ∼ 1020 ∼ 1019 0.36 1.4 – 0.3 1.1


Si (4 K) 4.22 × 1016 1.75 × 1016 0.1905 0.9163 – 0.153 0.537
Si (300 K) 2.8 × 1019 1.04 × 1019 0.19 0.98 – 0.16 0.49
Ge (4 K) 1.58 × 1016 8.24 × 1015 0.08152 1.588 – 0.0429 0.347
Ge (300 K) 1.04 × 1019 6 × 1018 0.082 1.64 – 0.044 0.28
CdSe 2 × 1018 – – 0.13 0.45 –
CdTe 7.5 × 1017 1.8 × 1019 – – 0.11 0.13 ∼0.8
CZT
GaAs 4.7 × 1017 7 × 1018 – – 0.067 0.45 0.82
GaSe
HgI2
InP 5.7 × 1017 1.1 × 1019 – – 0.077 0.089 0.6
PbI2
SiC (3C) 1.5 × 1019 1.9 × 1019 0.677 0.247 0.6 1.5
SiC (4H) 1.8 × 1019 2.1 × 1019 0.33 0.42 0.66 1.75
SiC (6H) 8.8 × 1019 2.2 × 1019 2.0 0.48 0.66 1.85
TlBr

detection. There are special materials that react to neutrons, which can be adapted if neutron detection is
the goal, or should be avoided if neutron discrimination is desired. One such semiconductor material is CdTe
(and CdZnTe), which offers good gamma-ray detection, but also reacts to low energy neutrons to produce
prompt gamma-rays. Special attention to material selection should be applied to low-energy gamma-ray and
x-ray detection, for which the K absorption edge may become important. For example, as seen in Fig. 16.1,
the total photon absorption coefficient below the two K edge energies of CdTe drops below that of Ge; hence
the lower Z material actually performs better than the higher Z material at energies below 26.727 keV. Si
is generally selected over Ge for characteristic x-ray analysis because its K edge is at a lower energy (1.840
keV) than Ge (11.115 keV); hence, the transition K edge has less effect on the photon absorption efficiency.
The mass density is of obvious importance, because increased mass density generally indicates higher
electron density. Further, photoelectric absorption is a strong function of Z; hence, the interaction efficiency
is strongly influenced by the atomic density of the highest Z component. Selection of materials with at least
one high Z component is important for gamma-ray detection. For instance, InP has one component with a
relatively high atomic number ZIn = 49, and one relatively low atomic number ZP = 15. Overall, the gamma-
ray absorption characteristic is predominately influenced by the density of indium because the phosphorus
component makes little contribution. Atomic number and mass density for several semiconductors are listed
in Table 16.2.

16.2.2 Band Gap


The energy band gap of a semiconductor Eg , introduced in Sec. 12.2.5, is
NC NV
Eg = kT ln (16.1)
n2i
or, more traditionally, is described by

ni = NC NV e−Eg /2kT , (16.2)
where ni is the intrinsic charge carrier concentration, NC is the effective density of state in the conduction
band, NV is the effective density of states in the valence band, k is Boltzmann’s constant, and T is the
710 Semiconductor Detectors Chap. 16

Figure 16.1. The linear attenuation coefficients for several representative


semiconductors.

absolute temperature. The relationship between ni and Eg is of major importance because a small increase
in the band-gap energy has a significant effect upon the free charge carrier concentration. Hence, to reduce
leakage current, it is desirable to use semiconductors with relatively large band-gap energies. Note that
lowering the temperature also reduces the value of ni , a method often used to suppress leakage current for
semiconductors that have relatively small values or Eg .
For most semiconductor radiation detectors, indirect band gaps are preferred over direct band gaps
mainly because the charge carrier lifetimes are theoretically much longer [Shockley and Read 1952; Hall
1952, 1959; Varshni 1967]. The reason for the difference is that electrons in the conduction band of an
indirect band-gap semiconductor must change in both momentum and energy to recombine with a hole,
whereas electrons in the conduction band of a direct band-gap semiconductor need only to lose energy to
complete the recombination process. Consequently, indirect band-gap semiconductors generally have higher
carrier extraction factor values than direct band-gap semiconductors for similar detector dimensions. Listed
in Table 16.3 are band-gap energies and types (indirect or direct) for several semiconductors used in radiation
detection. Note that the defect and impurity density of a semiconductor, if significant, can have a greater
effect on the overall mean free lifetime rather than the type of band gap.

16.2.3 Ionization Energy


A property strongly influenced by the energy band gap is the average ionization energy w, which limits
the minimum spectral energy resolution. For materials and detectors that suffer little to no charge carrier
trapping losses, the expected variance in charge pair excitation should follow Gaussian statistics so that

2 F Eγ
σN 0
= = F N0 , (16.3)
w

where F is the semiconductor Fano factor and Eγ is the energy of the radiation quantum. The resulting pulse
height spectrum, representing full energy peaks of radiation quanta, should also have a Gaussian appearance.
Sec. 16.2. General Semiconductor Properties 711

Hence, the full width at half maximum (FWHM) of these Gaussian peaks is, in terms of charge pairs N0 ,

Γ = FWHM|N0 = 2 [2 ln(2)]1/2 σ, (16.4)

which is transformed into units of energy by multiplying by w = Eγ /N0 as


1/2
F Eγ 1/2
Γ = FWHM|eV = 2w 2 ln(2)  2.355 [wF Eγ ] . (16.5)
w
This result can be written in terms of percent energy by dividing Eq. (16.5) by Eγ
1/2 1/2
2 [2 ln(2) wF Eγ ] wF
Γ = FWHM|% = 100  235.5 . (16.6)
Eγ Eγ

It becomes clear from Eqs. (16.5) and (16.6) that w significantly affects Γ and a small value of w is desirable.
The dependence of w upon the band-gap energy was studied by Klein [1968], and it was determined that
energy was expended by three mechanisms, namely (1) excitation across the band-gap energy, (2) residual
kinetic energy of excited charges, and (3) optical phonon losses. It is obvious that the minimum energy
required to produce an electron-hole pair must be Eg . Yet, the energy released from Coulombic interactions
of primary excited electrons, from either charged particle or gamma-ray interactions, can excite energetic
electrons from deep in the valence band or lower tightly bound energy bands. Further, the energy absorbed
may be more than required to transition the band gap into the conduction band. This excess energy is
manifested as kinetic energy of the charge carriers. If this excess kinetic energy is less than Eg , then it
becomes expended in the material and does not contribute to additional electron-hole pair creation.
The average ionization energy can be represented by

w = Eg + WL , (16.7)

where WL  is the average energy expended for purposes other than electron-hole production. Klein [1968]
breaks WL  into two fundamental components

WL  = ER  + EK , (16.8)

where ER  represents optical phonon losses and EK  represents thermalization losses. Optical phonons are
out of phase movements of the crystalline lattice and can be produced by energetic charged particles having
sufficient energy to excite electron-hole pairs. Their average energy is

ER  = r(ωR ), 0.5 eV ≤ r(ωR ) ≤ 1.0 eV, (16.9)

where r represents the average number of phonons per electron-hole pair created and ωR is the angular
frequency of optical phonon oscillations. Hence, ωR represents the energy per phonon (Raman quanta).
From experimental data of several semiconductors,5 Klein [1968] estimates a threshold for secondary
ionization as
3
EI  Eg (16.10)
2
and the average residual kinetic energy of excited charge pairs as

EK   2LEI = 3LEg , (16.11)

5 Klein [1968] lists Ge, Si, GaAs, InP as the sources of data.
712 Semiconductor Detectors Chap. 16

Figure 16.2. The average ionization energy (w) of several


semiconductors as a function of the band-gap energy (Eg ).

where L is a dimensionless scaling constant.6 Klein [1968] assigns a value of L = 3/5, yielding EK  =
(9/5)Eg , slightly below the minimum energy required to excite two electrons across the band gap. Klein
[1968] thereby produces the following formulation for the average ionization energy:

14
w= Eg + r(ωR ). (16.12)
5

Lund et al. [1988] and Shah et al. [1989] note that there appear to be two salient linear dependencies, both
following Eq. (16.12) as shown in Fig. 16.2, but having different ordinate intercepts.7 Using literature values
of w, a linear least squares method yields an ordinate intercept of r(ωR ) = 0.718 for the upper (traditional)
dependence. The ordinate intercept for the lower second dependence is found to be r = −1.467. The use of
r(ωR ) = 0.718 is within the limits of Klein’s theory and therefore has physical significance. However, as
pointed out by Owens and Peacock [2004], the use of r = −1.467 for the lower dependence does not follow
the theory of Klein [1968] and is used strictly as a curve fitting parameter.

6 This dimensionless scaling constant refers to the average wasted residual kinetic energy described in Van Roosbroeck’s [1965]
paper on“crazy carpentry”.
7 This discovery seems to have been missed by Alig and Bloom [1975], although it now seems obvious from their data.
Sec. 16.2. General Semiconductor Properties 713

16.2.4 Mobility
As discussed in Sec. 12.5, the charge carrier mobility is a strong function of the curvature of the energy
bands. Rapid charge carrier extraction reduces trapping and dead time problems and is fundamentally
dependent upon the charge carrier drift mobilities. Recall also from Sec. 12.5.1 that the charge carrier
mobility is inversely proportional to the charge carrier effective mass, and the effective mass is related to the
E-k diagram band curvature by
−1
d2 E
m∗ ∝ . (16.13)
dk 2
The curvature at the minima of the conduction band for most semiconductors is larger than the curvature
at the valence band maxima. Consequently, electron mobilities are almost always much larger than the hole
mobilities in a semiconductor. A few methods of measuring the charge carrier mobility of both electrons and
holes are described in the Sec. 15.4.5.
Also discussed in Sec. 12.5, the mobility tensor sums to a constant value for cubic crystals regardless of
the electric field force vector direction. However, this convenient condition does not necessarily hold true
for non-cubic lattice systems, and mobilities can be quite different depending on the electric field direction.
The mobility symmetry makes cubic crystals generally more desirable for radiation detectors than non-cubic
crystals.
Mobility decreases as the probability of charge carriers encountering motion impeding collisions increases.
Sources of motion impeding collisions include phonon (lattice) scattering (μl ), ionized impurity scattering
(μi ), neutral impurity scattering (μn ), crystal defect scattering (μD ), ionized deep donor and deep acceptor
scattering (μdi ), carrier-carrier scattering (μcc ), and piezoelectric scattering (μp ). Phonon scattering refers to
collision events caused from lattice vibrations of thermally excited lattice atoms. Ionized impurity scattering
refers to collisions from coulombic interactions between ionized impurities and charge carriers. Neutral defect
scattering becomes important at low temperatures and in polycrystalline materials. Piezoelectric scattering
is important in piezoelectric materials (for instance, GaAs and CdTe), in which displacement of atoms from
their lattice sites produces an internal electric field. Carrier-carrier scattering, in which charge carriers
scatter off each other, is important for high carrier densities, which is usually not the case for most radiation
detector applications. The resulting mobility is
−1
1 1 1 1 1 1 1
μ= + + + + + + + ... . (16.14)
μl μi μn μD μdi μcc μp
Of the many possible scatter mechanisms, the most influential on mobility are phonon scattering and
ionized impurity scattering. The mobility dependence of phonon scattering (μl ) is described by [Bardeen
and Shockley 1950] √
8πqe 4 C11
μl = , (16.15)
3Eds (m∗ )5/2 (kT )3/2
where C11 is the average longitudinal elastic constant of the semiconductor and Eds is the band-edge dis-
placement per unit dilation of the lattice from vibrational motion, and m∗ is the charge carrier effective
mass. Eq. (16.15) shows that phonon (lattice) scattering decreases mobility with increasing temperature and
effective mass. The mobility dependence of ionized impurity scattering is [Conwell and Weisskopf 1950]
√ $   2 /−1
64 π2s (2kT )3/2 12πs kT
μi = ln 1 + , (16.16)
Ni qe3 (m∗ )1/2 qe2 (Ni )1/3

where Ni is the ionized impurity concentration. From this result it is clear that increasing the impurity
concentration reduces mobility, typically becoming significant at ionized impurity densities greater than
714 Semiconductor Detectors Chap. 16

Figure 16.3. The mobility of Si and Ge as a function of impurity concentra-


tion at 300 K. Data are from Prince [1953] and Jacoboni et al. [1977].

1015 cm−3 as can be seen in Fig. 16.3. Notice also from Eq. (16.16) that the mobility from ionized impurities
decreases as T decreases. Hence, μl decreases with increased T while μi increases with increased T . Hence,
the overall dependence of mobility on temperature can be approximated by
−1
1 1
μ≈ + . (16.17)
μl μi
The general expression for charge carrier group velocity at relatively low electric fields is


vg  = μE, (16.18)
low E

where the mobility μ is an intrinsic property of the semiconductor. Hence, it becomes clear that large
mobilities are desirable for rapid charge carrier extraction from the detector. At high electric fields, the
charge carrier group velocity for many indirect band-gap semiconductors can be modeled as [Sze 1981]

 1
1/β
vg  = vs , (16.19)
high E 1 + (Eo /E)β

where vs is the saturation velocity at high electric fields and both Eo and β are experimentally determined
constants.
The simple empirical model of Eq. (16.19) does not take into account the crystal orientation, which does
in fact affect the charge carrier velocity (see Figs. 16.4 and 16.5). Indeed, under equilibrium conditions the
total effective mass tensor is constant regardless of electric field direction; however, at high electric fields the
charge carrier distribution in the transverse and longitudinal conduction band energy ellipsoids does change,
depending on the force vector of the electric field (Jacoboni et al. [1977]). Consequently, the effective mass
tensor also changes, and the charge carrier velocity characteristics are slightly different for electric fields
applied in different crystal directions.
Sec. 16.2. General Semiconductor Properties 715

Figure 16.4. The charge carrier velocities of Si as a function electric field and temper-
ature (77 K and 300 K). Data are from Jacoboni et al. [1977].

Figure 16.5. The charge carrier velocities of Ge as a function electric field and tem-
perature (77 K and 300 K). Data are from Reggiani [1978] and Jacoboni et al. [1981].
716 Semiconductor Detectors Chap. 16

Figure 16.6. The charge carrier velocities of GaAs, InP, and CdTe as a function electric
field at 300 K. Data are from Ruch and Kino [1967], Dalal et al. [1971], Canali et al.
[1971a, 1971b], Smith et al. [1980], Blakemore [1982], and González Sánchez et al. [1992].

There are a few semiconductors in which more than one conduction band minima can play a part in
electron transport. For instance, GaAs, InP, and CdTe are direct band-gap semiconductors, yet also have
indirect band-gaps that can accept electrons at high enough electric fields, and these indirect band gaps
have larger electron effective masses than their corresponding direct band gaps. Consequently, the high
electric field velocity for direct band-gap semiconductors, in which electron transfer to upper indirect bands
is possible, is much more complicated than given by Eq. (16.19) (see, for example, Pozela and Reklaitis
[1980]), and must take into account the change in effective mass for the upper valley minima. Hence, at
low voltages, the velocity is defined by the direct band-gap minimum, at medium voltages the velocity is
defined by a sharing of mobilities between the direct and indirect band-gap minima, and at high electric
fields the mobility is determined by one or more indirect band-gap minima. The sharing of electron mobility
between conduction band minima produces a region of negative differential resistance [Sze 1981], in which
the electron velocity and, consequently, the electrical current decrease with increased applied voltage (see
Fig. 16.6). A side effect of the negative differential resistance is to produce an instability, the Gunn effect,
that can produce oscillations at high voltage [Gunn 1963].

16.2.5 Resistivity
High resistivity for a material is important to reduce thermally generated current and other forms of leakage
current. For pure materials, the resistivity is mainly a function of band-gap energy. Examples include high-
purity Ge and float-zone refined Si. However, with a few exceptions, the purification of most compound
semiconductors is difficult. Consequently, high resistivity compound semiconductors are usually produced
through compensation methods (as outlined in Sec. 12.5.4). The natural resistance of a semiconductor block
Sec. 16.2. General Semiconductor Properties 717

can be described by
ρL L
R= = , (16.20)
A qe A(nμn + pμp )
where L is the length of the block, A is the area of each electrical contact at the ends, n is the free electron
concentration, p is the free hole concentration, μn is the electron mobility, and μp is the hole mobility. An
impulse current should be significantly higher than the background leakage current.
The type of detector contacts required is strongly influenced by the material resistivity. If the resistivity
is  5 × 1010 Ω-cm, a resistive device, or photoconductor, can be fashioned. If the resistivity is below
5 × 1010 Ω-cm, it is usually best to construct a junction diode, as described in Sec. 15.3.1 (and in Sections
15.3.2 and 15.3.3), to suppress electronic noise from leakage currents. There are methods to increase the
resistivity of a semiconductor with compensation methods, but there are physical consequences that can
arise from the operation of junction diodes fabricated from compensated high-resistivity materials and are
addressed later in this chapter.

16.2.6 Mean Free Drift Time


The recombination time τr is the average lifetime of an electron before it recombines with a hole, whereas
the mean free drift time τm is the average time a charge carrier is in motion before it encounters a physical
impediment that stops its motion. In a pure defect-free semiconductor, the recombination time is essentially
the same as the mean free drift time. However, they are not the same in most semiconductors, mainly
because recombination is usually assisted by transitions through band-gap defect states.
The lifetime of a charge carrier is largely a function of the band-gap energy and defect density. Hall
[1959] and Varshni [1967] show that the recombination time for indirect band-gap semiconductors can be
significantly longer than that observed for direct band-gap semiconductors. The fundamental reason for the
difference is electrons must lose energy and change momentum to transcend the band gap to recombine with
a hole; however, electrons in a direct band gap need only to lose energy to recombine with a hole. The
recombination times predicted by either Hall [1959] or Varshni [1967] are relatively long by comparison to
observed values. This difference is explained by the theory of Shockley and Read [1952] and Hall [1952],
which attributes recombination mainly to the trap density in a semiconductor.
Ultimately, it is the mean free drift time that affects the performance of a semiconductor detector, and it
is τm that is usually measured to determine the often quoted μτ product. Recall from Sec. 15.5 that charge
carrier collection is directly related to the μτ product, in which the carrier extraction factor for a planar
detector is given by Eq. (15.221), namely,
μτm E(x)
= , (16.21)
W
where W is the detector width. Sufficiently good energy resolution is observed if both carrier extraction
factors are greater than 50. The value of  for holes and electrons can be increased by reducing W or
increasing E(x). However, τm is an intrinsic property of the material, increased only by improving the
crystal quality. Semiconductor materials with relatively large mean free drift times are generally sought for
semiconductor spectrometers.

16.2.7 Linearity
The process by which information carriers are produced in semiconductors differs from scintillators and gas
detectors. In Sec. 12.3 it was shown how the electron energy states in solids form a quasi-continuum of energy
bands and energy gaps. As discussed in Chapter 4, charged particles interact in a medium primarily through
Coulombic interactions while photons may interact by several different processes, usually the photoelectric
effect, Compton scattering, or pair production (if Eγ > 1.022 MeV). These initial electrons excited from
718 Semiconductor Detectors Chap. 16

Figure 16.7. Shown are dimensionless measures of the pulse height defect
(Δ) vs. dimensionless energy (0 ) of heavy ions absorbed in Si and Ge.
The dotted line is hypothetical limit of the expected charge production, where
Δ = 0 . Data are from Haines and Whitehead [1966].

lower bands are either removed from the nucleus (ionization) transferred to the upper bands (excitation),
and electrons with sufficient kinetic energy can ionize more free electrons (delta rays) that further excite
electrons. This process is common to both semiconductors and scintillators.
Scintillators rely on electrons transitioning through energy states to produce photons subsequently de-
tected by a light sensitive device. However, in a semiconductor, the free electrons are measured directly by
the current they produce under an applied voltage, much like a gas-filled detector. For mature semiconduc-
tors with relatively long charge carrier mean free pathlengths, and large μτ products, the measured current
or charge is a linear function of energy deposition. Such is not the case for scintillators for which phosphor
saturation (organic scintillators), exciton losses (inorganics), or other competing mechanisms lead to non-
linear responses with respect to energy and particle type. Overall, the average number of electron-hole pairs
produced per unit energy in a semiconductor is remarkably linear over a wide energy range.
However, there are some situations that can produce a non-linear output from a semiconductor. For
instance, the active thickness of the detector must be capable of absorbing the total energy deposited by an
ionizing particle. If the ionizing particle range extends beyond the active region range, then some energy is
lost and the resulting signal is diminished. The probability of this form of non-linearity increases with particle
energy. For low-energy charged particles, the dead layer surrounding a detector absorbs energy, resulting
in energy loss and some amount of energy non-linearity in the output. Charge carrier trapping can also
cause the appearance of a non-linear spectrum. Although Si and Ge detectors tend not to suffer much from
trapping effects, compound semiconductors almost always do. Hence, it is common to irradiate the cathode
of compound semiconductors in order to emphasize electron charge induction over hole charge induction.
Still, the average charge measured per unit energy deposited reduces with increasing particle or photon
energy, typically degrading the energy resolution. For heavy ions, the dense charge cloud produced can
cause appreciable recombination, which can also contribute to non-linear output. Recombination problems
can be reduced by increasing the detector operating voltage.
Also, heavy ions can lose energy by direct nuclear collisions, which do not produce electron-hole pairs
[Lindhard and Nielsen 1962; Haines and Whitehead 1966]. Consequently, there can be appreciable non-
Sec. 16.3. Semiconductor Detector Applications 719

linearity in the number of electron-hole pairs produced from heavy low-energy charged particles. The average
dimensionless energy losses Δ as a function of dimensionless energy 0 for a few heavy ions interacting in
either Si or Ge are shown in Fig. 16.7. The greatest fraction of energy loss occurs at 0 values less than 10,
corresponding to approximately 6 MeV for I ions, 3 MeV for Br ions, and 400 keV for Si ions interacting in
Si [Haines and Whitehead 1966]. The dashed line indicates the situation in which all energy is lost to nuclear
non-ionizing recoil events. Below 0 = 5 nearly half of the ion energy is lost to recoils, and the situation
asymptotically approaches the hypothetical limit with decreasing 0 .

16.3 Semiconductor Detector Applications


Briefly described are common radiation detection applications that employ the use, at times, for semiconduc-
tor radiation detectors. In most cases, these applications exploit the low ionization energy of semiconductors
to produce radiation spectrometers, and semiconductors are used to detect charged particles, energetic pho-
tons, and neutrons. Some systems use the semiconductor properties to make electronic devices and arrays
into compact low-power detectors. Some details on specific types of semiconductor detectors are provided
as later sections.

16.3.1 Charged Particle Detectors


Semiconductor charged particle spectrometers offer high energy resolution for energetic ions. Typically, the
devices are operated in vacuum, along with the source, to eliminate energy losses from a charged particle
as its passes from the source to the detector. The detectors are typically designed with thin contacts
and/or thin pn junctions in order to reduce particle energy loss in the non-sensitive (or dead) region of the
contact. Because low Z elements have less problems with ion backscattering, Si is typically the material
choice for particle detectors. These detectors can be used for a variety of charged particle identification and
characterization purposes, including high resolution spectroscopy of α particles, β particles, protons, and
heavy ions, continuous air monitoring, and particle telescopes.
Spectroscopy requires that the full energy of the particle be deposited in the active region of the detector,
hence charged particle spectrometers are constructed in such a manner that the depleted region extends
beyond the range of the particle under investigation. For most alpha particle spectroscopy applications, a
depletion width of 100 microns is adequate. Proton ranges are much longer than those of alpha particles of
the same energies, and special detectors that can achieve wider depletion widths may be required. Electrons
generally have longer ranges in semiconductors than heavy ions, but also have higher backscatter coefficients.
There are some particle detectors designed for the detection of minimium ionizing particles (MIPs). Note
that by definition MIPs can be β particles, protons or any other ionizing charged particles, provided that
their kinetic energy is at least twice their rest mass energy. For electrons and β particles, they are classified
as MIPs if their kinetic energy exceeds 1.022 MeV. For protons, they must exceed 1.88 GeV energy to be
classified as MIPs.
β particles are emitted from a radioactive source with a continuous energy spectrum (see, for example,
Fig. 3.20) and, thus, do not have discrete energy peaks in the pulse height spectrum. Further backscattering
and self-shielding can often distort the measured spectrum. Because MIPs tend to deposit an even distribu-
tion of energy with distance (dE/dx is constant), detectors for MIPs are designed to detect a fraction of the
particle energy (ΔE) rather than the total energy. Hence, they are commonly designed to absorb enough
energy to identify a MIP, but usually not all of the MIP energy.

16.3.2 Gamma-Ray and X-Ray Detectors


Semiconductors excel above gas-filled and scintillators as energy spectrometers. This nearly universal prop-
erty is a consequence of the lower ionization energy that allows the excitation of a greater number of charge
720 Semiconductor Detectors Chap. 16

carriers (electron-hole pairs) per unit energy than in gas-filled or scintillation detectors. By pure Gaussian
statistics, the fractional standard deviation is smaller for semiconductors than other detectors. Further,
with few exceptions, the Fano factor is smaller for semiconductors than gases and scintillators. Recall from
Sec. 6.8.1 that the FWHM of a Gaussian distribution is

FWHM = 2 2 ln(2)σ 2  2.355σ, (16.22)

and conversion of this result to the number of charge pairs is done by inserting the Fano factor correction
so that the energy resolution is 
2 ln(2)Eγ F
FWHM = 2 . (16.23)
w
This number is easily converted to units of energy by multiplying Eq. (16.23) by the semiconductor average
ionization energy (w), so that

FWHM(energy) = 2 2 ln(2)Eγ wF  2.355 Eγ wF . (16.24)

Indeed, the standard for reporting energy resolution for semiconductors is in terms of energy, commonly in
units of keV. This standard is different for scintillators, in which the FWHM is usually reported as a percent
of the gamma-ray energy. The main reason for the change from the traditional standard used for scintillators
is the exceptional energy resolution of semiconductors, commonly sub-percent for Si and Ge semiconductors.8
Note the energy resolution of a semiconductor detector is expected to increase with the square root of the
gamma-ray energy, a dependence that holds relatively well for Si and Ge detectors. However, trapping effects
cause the full energy peak to appear non-Gaussian for most compound semiconductors, and Eq. (16.24) is
usually not a good predictor of the FWHM.
Semiconductor gamma-ray detectors are usually smaller than their scintillator counterparts, and it is
common for a semiconductor detector spectral response to have a relatively high Compton continuum in
the spectrum. This problem has been addressed by manufacturing large semiconductor detectors (there are
rather sizeable Ge detectors available in the commercial market for high cost), or by producing detectors
from large Z materials to improve gamma-ray absorption. However, the improved energy resolution typical
of semiconductor detectors is usually enough to permit easy identification of gamma-ray full energy peaks
and any additional spectral features (such as escape peaks).
The compactness of semiconductors accompanied by the generally high energy resolution makes them
attractive radiation detectors. Further, they do not have a secondary detection device, such as a photo-
multiplier tube or a SiPM array required to properly operate a scintillation detector. Overall, scintillators
are often used when modest energy resolution is acceptable and semiconductors are used when high energy
resolution is most important. Note also that semiconductor devices can be fashioned into arrays and elec-
tronic readout that can identify the location of where the interaction occured in the detector volume, an
advantage not easily duplicated with scintillation detectors. These advantages allow the production of direc-
tionally sensitive gamma-ray detectors, either as physical arrays composed of many individual detectors or
as pixelated devices with sophisticated electronics that localize events in a semiconductor block. A variety of
semiconductor gamma-ray detectors, commercial and experimental, fabricated from different materials are
described throughout the remainder of this chapter.

8 Inrecent times, energy resolution for compound semiconductor detectors, such as CdZnTe and HgI2 , is often reported in terms
of percent. However, this departure from an established system is not strictly correct, and is an unfortunate consequence of the
deleterious effect that crystal imperfections and charge carrier trapping have on energy resolution, causing many compound
semiconductors to perform with similar energy resolution as the best scintillators.
Sec. 16.3. Semiconductor Detector Applications 721

16.3.3 Neutron Detectors


Semiconductor radiation detectors used as neutron detectors are neutron reactive film
typically configured as pn-junction or Schottky-junction diodes
coated with a neutron reactive material. The basic construction
of such a detector is shown in Fig. 16.8, in which a Schottky or pn reaction
product V+
junction diode detector has a coating of neutron reactive material
neutron
applied to the surface. Typically the devices have either 10 B or
6
LiF as the active coating. The absorption cross sections for both A
10
B and 6 Li follow a 1/v dependence. The 10 B(n,α)7 Li neutron re-
action yields two possible de-excitation branches from the excited electron-hole
11
B compound nucleus, namely reaction pairs
product

⎨ 42 He (1.4721 MeV) + 73 Li∗ (0.8398 MeV) [93.7%]
0 n+ 5 B −→
1 10
⎩ 4 He (1.7762 MeV) + 7 Li (1.0133 MeV) [6.3%], semiconductor
2 3

where the Li ion in the 94% branch is ejected in an excited state, Figure 16.8. Cross section of a coated semi-
which deexcites through the emission of a 480-keV gamma ray. conductor neutron detector.
Fully enriched 10 B has a microscopic absorption cross section for thermal neutrons (2200 m/s) of 3840 barns.
With a mass density of 2.15 g cm−3 , the solid structure of 10 B has a macroscopic thermal absorption cross
section of 500 cm−1 .
The 6 Li(n,t)4 He neutron reaction yields a single product branch,
1
0n + 63 Li −→ 31 H (2.7276 MeV) + 42 He (2.0553 MeV).

The reaction products from the 6 Li(n,t)4 He reaction are more energetic than those of the 10 B(n,α)7 Li
reaction and, hence, are much easier to detect and discriminate from background radiations. 6 Li has a
relatively large microscopic thermal neutron absorption cross section of 940 b, although it is less than that
of 10 B. Unfortunately, Li is a chemically reactive metal, and, therefore, it is the stable compound 6 LiF, with
a 2200-m/s macroscopic cross section of 57.51 cm−1 , that is usually used as the reactive coating.
For thermal neutrons, the charged particle reaction products are ejected in opposite directions, meaning
that only one reaction product can actually enter the semiconductor detector. Further, the reaction products
lose energy as they pass through the neutron absorber to the semiconductor detector, thereby limiting the
effective absorber thickness. Detectors of this type are limited to less than 5% thermal neutron detection
efficiency. These devices are generally not commercially available as independent units; rather they are sold as
an active component inside some electronic dosimeter modules. Advanced versions of coated semiconductor
detectors, having etched features backfilled with neutron reactive materials, have reported efficiencies greater
than 65%. A detailed discussion on these advanced coated-semiconductor neutron detectors is in Chapter
17.
There have been attempts to use semiconductors in which at least one type of constituent atom is neu-
tron reactive. Semiconductors with neutron reactive isotopes that promptly emit charged-particle reaction
products include B-based semiconductors (such as BC4 , BN, BP, and BAs) and Li-based semiconductors
(such as LiZnP, LiZnAs, and LiInSe2 ). Semiconductors with neutron reactive isotopes that promptly emit
gamma-ray reaction products include Cd-based semiconductors (such as CdTe and CdZnTe) and Hg-based
semiconductors (such as HgI2 ). The concept is simple; neutrons interact with the reaction isotopes that
promptly emit ionizing radiation back into the semiconductor. The ionizing radiation produces electron-
hole pairs in the semiconductor, and these charges are drifted with an electric field to produce an induced
current or induced voltage on an electronic output. To date, these types of neutron detectors have been
722 Semiconductor Detectors Chap. 16

Figure 16.9. The theoretical energy bands of Si at 300 K calculated with a


pseudopotential method. Data are from Chelikowsky and Cohen [1976].

largely unsuccessful. Regardless, a section in Chapter 17 is reserved for discussion on these types of neutron
detectors.

16.4 Detectors Based on Group IV Materials


The family of semiconductor materials based on group IV materials include Si, Ge, diamond, and SiC. Both
Si and Ge detector processing are mature technologies, having been developed as semiconductors for electron
devices for over 50 years. By far, most semiconductor radiation detectors are fabricated from either high-
purity Si or Ge, although there is a modest market for other semiconductor detector materials. Diamond is
also used as a radiation detector material, but its low value of Z diminishes its effectiveness as a gamma-ray
detector. Hence, diamond is mainly explored for used as a charged particle detector. SiC is also a group
IV material, but it is also a compound semiconductor, which can suffer from intrinsic defects (antisites, for
instance) typically not a problem with Si, Ge, or C (diamond) crystals. The processes by which diamond
and SiC are produced increase the material costs, hence these materials are used only in cases in which
alternative semiconductors are inadequate. For instance, both diamond and SiC can be used in higher
temperature environments than Si or Ge, and both diamond and SiC tend to have higher radiation hardness
than either Si or Ge. Basic detectors fashioned from these semiconductor materials are described in following
subsections.

16.4.1 Detectors Based on Silicon


Silicon is by far the most studied of the semiconductor materials for electronic devices, and it is popular
for its many beneficial physical and electronic properties. As can be seen from Fig. 16.9, the energy of
the band gap for Si is 1.12 eV, which is just wide enough for room temperature operation of small volume
devices. Further, the band gap is indirect, and charge carrier mean free drift times are relatively long for
highly purified material. The density of Si is only 2.33 g cm−3 and it has an atomic number of 14, low
for most gamma-ray detector applications, but still useful as an x-ray and low-energy gamma-ray detector.
The average ionization energy of Si is 3.6 eV per e-h pair with 0.115 as the Fano factor. The backscatter
Sec. 16.4. Detectors Based on Group IV Materials 723

coefficient of Si is relatively small, making it a good choice for charged particle spectrometers. It has a
native oxide (SiO2 ) that is robust, stable, and electrically and thermally resistant. The production of thicker
SiO2 layers is straightforward, easily grown through ‘dry’ and ‘wet’ processes at high temperature (> 950◦ C)
in a tube furnace. The crystal has a cubic FCC lattice structure.9 Recalling from Sec. 12.5, the average
charge carrier mobility is practically constant regardless of charge carrier direction. It is easily etched by
wet and dry processes, which include anisotropic and isotropic methods. Doping is straightforward, and can
be performed with thermal diffusion and ion implantation. Because of its high melting point of 1414◦C,
activation of these dopants is also straightforward by many methods, including rapid thermal annealing and
furnace annealing. Si is notably a material that can be doped through neutron activation, mainly because
30
Si + n → 31 Si (t1/2 = 2.62 hrs) → 31 P (16.25)

reactions lead to the production of stable phosphorus, an n-type dopant in Si. Uniformity is ensured by
the low thermal neutron absorption cross section of only 0.171 barns. Si is a relatively tough material,
with a Mohs hardness of 7, and it has high tensile strength. Si crystalline material can be acquired as
large diameter ingots and sizeable prepolished wafers. Electronic grade Si wafers can be acquired as 12-inch
diameter wafers or even greater for special cases. High purity float-zone-refined Si wafers of 6-inch diameter
can also be acquired commercially.
Charged Particle Detectors Based on Si
Charged particle detectors are designed with thin contact regions to minimize energy loss in the electrical
contact. Such energy loss can increase the variance on the measured energy, while reducing the total
integrated energy deposited within the detector active region. For semiconductors with small band gaps,
such as Si and Ge, thin rectifying contacts are fabricated as either Schottky barriers and shallow pn junctions.
The Schottky barrier design is perhaps one of the easiest semiconductor detectors to fabricate, requiring a
clean semiconductor surface upon which are applied select metals to form a Schottky barrier. These detectors
are commonly referred to as surface barrier detectors.10 Shallow pn junctions, prepared by diffusion or ion
implantation, require more process steps, but tend to be more robust with lower leakage currents than SSB
detectors.
The most commonly used semiconductor for charged particle detection is Si. Si possesses many physical
attributes that make it attractive as the select detector material, including low Z to reduce backscatter, a
strong and easy to grow high resistivity oxide layer, a relatively strong crystal structure with high tensile
strength, and chemical stability that enables a relatively straightforward fabrication of detectors. Further, Si
has an indirect band gap of 1.12 eV that produces long charge carrier lifetimes and allows room temperature
operation for detectors of conservative size.
Silicon surface barrier (SSB) detectors were amongst the earliest versions of practical semiconductor
radiation detectors, introduced in 1958 by Davis as alpha particle detectors. The simplistic construction
requires only a pristine etched Si surface upon which a gold layer is evaporated, forming a rectifying Schottky
barrier.
An etch commonly used for SSB detectors is CP4A,11 because it produces a pristine mirror finish on a
Si surface [Dearnaley and Northrop 1966]. High purity n-type or p-type Si is etched, mounted and epoxied

9 Often referred to as a ‘diamond lattice’, this identification is not one of the Bravais lattices. A diamond structure has two
identical atoms, a part of a tetrahedron, on each FCC lattice point.
10 The origin of “surface barrier” as a detector name is not exactly known by the authors; however, the earliest reference

discovered that uses this name is the 1955 Ph.D. dissertation by Simon.
11 CP4A is a 3:5:3 mixture of HF(48%):HNO (73%):CH COOH(100%) and must be kept in a plastic container (not glass). The
3 3
formula rapidly etches Si, and must be cooled (such as in an ice bath) to control the etch rate. This etch is excellent for
producing home-made SSB detectors, and leaves a pristine mirror finish if the samples are agitated during the etch process.
724 Semiconductor Detectors Chap. 16

ceramic ring oxide implanted p-type


Au contact passivation contact
epoxy

high purity Si high purity n-type Si


(n or p type)

epoxy
Al contact implanted n-type
contact
surface barrier detector ion-implanted detector
Figure 16.10. General configurations for Si surface barrier detectors and
implanted junction detectors.

into a ceramic ring. The samples are bonded into insulating collars with an amine-free epoxy and desiccated,
followed by evaporating a metal layer ranging from 80-200 nm thick on opposite surfaces, commonly Au on
one side and Al on the other. The thin contact region minimizes the amount of energy lost by particles that
enter the device, a necessary precaution to preserve high energy resolution.
At high voltages, it is common to have electrical breakdown at the perimeter of the diode, where the metal
crosses from the epoxy bead to the semiconductor surface (see Fig. 16.10). Introduction of an iodine-doped
amine epoxy around the perimeter atop the amine-free epoxy bead on the Au side (before evaporation) can
produce a reverse biased surface diode, which mitigates electrical breakdown [Gibbs 1988]. Addition of a
guard ring helps with the reduction of leakage current noise [Dearnaley and Northrop 1966]. Environmental
conditions can affect the performance of SSB detectors, mainly the ambient temperature and humidity. Mod-
ernized process methods help mitigate these problems, and include improved surface preparation methods
and the addition of a perimeter oxide around Si sample [Fretwurst et al. 1990].
These delicate surface barrier detectors can be easily damaged by improper handling and are often difficult
to clean. Detectors can be obtained in a variety of sizes, ranging from a few mm to 50 mm diameter. These
detectors are usually light sensitive and must be operated in darkness, although commercial companies do
offer versions that can operate in ambient light, at the expense of energy resolution. Depletion depths
range from approximately 100 microns up to, for special cases, 5 mm. A simple nomogram representing
the depletion width as a function of voltage and impurity concentration can be produced by linearizing
Eq. (15.61) [Allcock et al. 1963; Blankenship and Borkowski 1960],
  
1 2s Vbi − V
log10 (W ) = log10
2 qe Nb
or
1 1
log10 (W ) − log10 (2s μ) = [log10 (ρ) + log10 (Vbi − V )] , (16.26)
2 2
where Nb has been replaced with 1/qe μρ and the applied voltage V is negative (reverse bias). With the
properties for Si listed in Table 16.4, such a nomogram was developed for a silicon surface barrier detector,
shown in Fig. 16.11, in which the depletion width is a function of material resistivity (n-type and p-type).
Implanted junction detectors rely upon an abrupt junction pn diode for rectification (see Fig. 16.10).
These devices are often fabricated from high purity n-type Si. An oxide is grown on the devices for passiva-
tion, followed by etching windows back to the Si surface. Shallow p-type and n-type dopants are implanted
on opposite sides of the Si surface and thermally activated. An implanted junction of dopants, usually boron
into n-type Si, initially produces a Gaussian distribution displaced from the semiconductor surface by the
average ion range. These implants must then be electrically activated, usually through an annealing process,
Sec. 16.4. Detectors Based on Group IV Materials 725

Figure 16.11. The depletion region as a function of material


resistivity and reverse voltage for Si particle detectors. A straight
line will yield material resistivity (n or p type), the depletion depth
and applied voltage, according to Eqs. (15.61) and (15.64). The
example shown with the dotted line is for 5 kΩ n-type material at
50 volts reverse bias, which yields W = 282 microns.

which serves to also redistribute the dopants. It is typical to model the final doping distribution as an error
function (see Sec. 6.8.2). This implantation process produces a dead layer junction with a thicknesses of
about 50 nm that serves as the conductive contact so that there is no need for a metal overlayer. Because
there is no thin metalization layer over the detector, implanted junction detectors are more robust and easier
to clean than common SSB detectors. Implanted junction detectors can be used for the same basic detection
functions that SSB detectors are used. SSB and implanted junction detectors can be acquired in numerous
shapes, sizes and configurations, making them a versatile choice for particle detection and spectroscopy. Fur-
ther, the detectors can be acquired as multi-element arrays for position sensing and timing purposes. The
adaptation of very large scale integration (VLSI) processing technology to Si detectors allows detector arrays
to be fabricated in a vast number of detector designs, including custom devices contracted to commercial
vendors.
Both SSB and shallow junction pn diodes operate practically the same. Both rely on a reverse biased
rectifying junction to reduce leakage current, and the active region is a function of applied reverse voltage
and impurity concentration, as described in Sec. 15.3.1. In both designs, the rectifying contact is insensitive
726 Semiconductor Detectors Chap. 16

Figure 16.12. Room temperature alpha-particle differential pulse height spectra of spectroscopic grade
241 Am and 226 Ra sources taken with a 24-mm diameter implanted-junction Si detector operated in

vacuum.

to ionizing radiation, considered to be a “dead region”. Modern commercial implanted junction detectors
have slightly less dead region thickness, an indication, in principle, that they can achieve higher energy
resolution than an SSB detector. However, there are many factors that affect the overall energy resolution
and include detector area, reverse bias voltage, background impurities, leakage current, thickness uniformity,
and crystal orientation. Example alpha-particle spectra from a common commercial implanted-junction Si
detector are shown in Fig. 16.12.
The area of a charged particle detector, whether an SSB detector or ion implanted detector, directly
affects the capacitance as well as the depletion depth. Capacitance increases linearly with detector area and
decreases with depletion width. Consequently, high-purity float zone refined Si is required to achieve large
depletion depths at manageable operating voltages, as indicated by the nomogram of Fig. 16.11. The reverse
bias leakage current generally increases with applied voltage. Recall from Sec. 15.3 that the leakage current is
smaller for a pn junction than that of a Schottky barrier, the former being a function of the minority carrier
injection condition and the latter being a function of thermionic emission over a potential barrier. Hence, it
is expected that for a given detector area the implanted junction detector has a lower leakage current than
the SSB detector.
A type of Si particle detector, typically fashioned as an SSB detector, is a transmission device that allows
particles to transport all the way through the detector and out the opposite side. These ΔE detectors
measure only a fraction of the energy of a charged particle, and because the total energy deposited is a
function of the detector mass encountered, flatness and uniformity are important. The resolution of the
energy peak from a transmission device is largely dependent upon the total planar flatness of the detector.
For instance, a surface deviation of only 1% causes a similar deviation in energy resolution. Transmission
detectors can be acquired from commercial vendors with thicknesses less than 20 microns to over one or two
millimeters, and are designed to operate under full depletion conditions. Transmission detectors are used for
particle identification, time-of-flight measurements, backscatter experiments, and particle telescopes.

Example 16.1:
Assume that you have an SSB transmission detector with average thickness of 15.5 microns, and that
it has a thickness deviation from 14 to 15 microns across its thickness. The alpha particle source under
investigation is 241 Am, measured in vacuum. Assume that the average energy loss for an alpha particle
through 15.5 microns of Si is 15.5 eV/Å. How does this thickness deviation affect the energy resolution of
that transmission peak?
Sec. 16.4. Detectors Based on Group IV Materials 727

Solution:
The total energy deposited in the detector is,
  
15.5 eV 1 Å
E  15.5 μm = 2.403 MeV.
Å 10−4 μm
The total energy spread from the thickness variation is
  
15.5 eV 1 Å
ΔE  1 μm = 155 keV,
Å 10−4 μm
which is a 6.45% difference.

The crystal orientation is also important. The lattice of a semiconductor forms channels that ions can
travel through without suffering ionic collisions, an effect named channeling. For cubic semiconductors,
channels form as hexagons in the {110} directions, rhombuses (squares) in the {100} directions, and squares
in the {111} directions. Ions that enter into the surface below a critical angle with respect to normal
incidence, usually 6◦ or less, scatter down these channels so they penetrate deeply into the semiconductor.
To prevent a wide doping distribution depth from implantation, Si wafers are usually oriented beyond this
critical angle, and often 7◦ to 11◦ from normal is adequate. Otherwise, the implanted dopant can travel
much further into the semiconductor, thus causing a much thicker dead layer. The same is true for particle
detection. Consequently, SSB and implanted-junction detectors are commonly made with the flat surface
polished at an off angle to conventional [100], [111], and [110] directions. Performance data for implanted
and SSB Si detectors is given in Table 16.5.
Position Sensitive Particle Detectors Position sensitive detectors are devices that have the capability of
simultaneously sensing the absorbed energy and the location of the ionizing event. Semiconductor detectors

Table 16.5. Typical alpha-particle energy resolution of a few rep-


resentative commercially available semiconductor detectors. Many
other sizes are offered by the different vendors.
area energy FWHM
detector comments source*
(mm2 ) (keV) (keV)

implanted 5486 13 W = 100 μm


100 C,O
Si diode 5486 12 W = 500 μm
implanted 5486 17–21 W = 100 μm
450 C,O
Si diode 5486 15–19 W = 500 μm
implanted 5486 27–33 W = 100 μm
900 C,O
Si diode 5486 22–28 W = 500 μm
p-type 5486 15–17 W = 100 μm
50 O
SSB 5486 15–17 W = 500 μm
p-type 5486 16–19 W = 100 μm
150 O
SSB 5486 16–18 W = 500 μm
p-type 5486 30–40 W = 100 μm
900 O
SSB 5486 30–53 W = 500 μm
∗C = Canberra, O = Ortec.
728 Semiconductor Detectors Chap. 16

charge sensitive
preamplifier Au contact incident
particle
A
R -+
depletion region + -
-V - +
substrate region
charge sensitive
preamplifier
C electrical resistive electrical
contact contact contact
B
R
x L-x
L

Figure 16.13. The resistive divider position sensitive detector operation principle.

are often used as position sensitive devices because of compactness from VLSI process methods, low operating
voltages, and relatively high stopping power as charged-particle detectors. Double-sided cross strip detectors
can have spatial resolutions as low as 25 μm, and pixellated detectors can have spatial resolution as small
as 0.4 mm. Large arrays of position sensitive Si detectors can be used in collider facilities, x-ray scattering,
and Compton cameras. Drift diode configurations, a variant design that drifts electronic charge carriers
laterally along the detector to a small collection contact, offer low capacitances with large sensitive areas.
These detectors are available in many forms, with some of the more popular configurations described here.
Resistive Divider Detectors Resistive divider detectors operate on the same principle as their gas-filled
detector counterparts, described in Sec. 10.6.4. The detector consists of a rectifying contact in the form of
a long strip, typically a few millimeters wide and a few centimeters long [Clegg et al. 1966; Bock et al.
1966]. The rectifying contact may be a simple Schottky contact, or can be fashioned as a pn junction. A
conductive electrical contact, usually gold, is applied to the rectifying junction, and the detector is operated
under partial depletion. The back contact has two conductive contacts, one at each end, and a thin relatively
resistive contact (such as a layer of Bi, Cr, Ni, or Al) is applied between these two contacts [Bock et al.
1966; Bertolini and Coche 1968]. Because there are essentially three conductive contacts (see Fig. 16.13),
it inspired the original name of these devices as ‘nuclear triode detectors’. The literature suggests that
unannealed implanted surfaces perform better as resistive contacts than evaporated metal layers [Laegsgaard
et al. 1968; Elad and Sareen 1974], because the implantation process has superior uniformity and the lattice
damage produced by the implantation process increases the surface sheet resistance.
Although in depth analyses of the device operation are available in the literature [Kalbitzer and Melzer
1967; Alberi and Radeka 1976], the general operation of the detector can be simplified as follows. The detector
is operated with at least two charge sensitive preamplifiers. A reverse bias is placed on the rectifying contact,
which produces a depletion region. One of the bottom conductive contacts is grounded and the conductive
contact at the other end of the resistive region is connected through a second preamplifier. Ionizing events
that occur at position x produce a total induced charge on the upper preamplifier at position A in Fig. 16.13
proportional to the total absorbed energy (E) in the depletion region. However, the conductive contacts at
points B and C are affected by the distributed resistance of the lower contact. Consequently, the current
flowing to points B and C is divided by the fractional resistances represented for lengths L-x and x. From
Ohms law
x EA RC
EB = EA = , (16.27)
L RC + RB
where L is the length of the bottom resistive contact, and RC and RB represent the resistances of lengths x
and L-x, respectively. To find the linear position of the initial ionizing event, one needs to divide only the
output from location B by the output of the upper preamplifier at location A, i.e., x = LEB /EA .
As simple as the concept is, these position sensitive detectors can provide a spatial resolution of about
30 μm FWHM at room temperature, reducing to 10 μm at 77 K [Elad and Sareen 1974]. Further, this type
Sec. 16.4. Detectors Based on Group IV Materials 729

top surface readout


semiconductor

top metallization
bottom surface readout

electrodes

bottom oxide
electrodes s
on
n-type junctions cti
jun
e
p-type Si material typ
p-
metallization

oxide

Figure 16.14. Basic structure of a cross-strip position sensitive particle de-


tector. (left) Top view of the readout pattern and (right) isometric view of the
basic construction.

of detector can be fashioned as an x-y position sensitive detector by aligning numerous parallel strips, for
which the resistive divider identifies the x location, and the strip number identifies the y position. Spatial
resolution of approximately 0.2 mm FWHM was reported for one such device [Lamport et al. 1976].

Double-Sided Cross-Strip Detectors Introduced originally by Hofker et al. in 1966, the dual-sided
cross-strip detector has orthogonal conductive strips applied to opposite sides of a semiconductor substrate.
From the top view depiction of Fig. 16.14, it is easy to understand the original name given by Hofker et
al. [1966] as ‘checker board counters’. These detectors are designed to operate under full depletion, with
one side of the device having rectifying contact strips and the other side having orthogonal ohmic contact
strips. The readout scheme becomes obvious by simple inspection. Ionizing events that occur within the
detector produce electron-hole pairs. Electrons are swept to the anode strip in closest vicinity and the holes
are swept to the closet cathode strip. Consequently, an ionizing particle produces an induced current pulse
through the leads of one of the front strips and of one of the back strips. The event location is identified
on the x-y grid because the opposing signal strips overlap. The scheme requires at least one preamplifier
for each strip on the front and back. It its simplest form, a cross-strip detector can be manufactured by
applying conductive contacts to opposite sides of various semiconducting of semi-insulating substrates, such
as Si, Ge, GaAs, CdTe, CdZnTe, and HgI2 . For most applications, Si is a preferred choice.
A method to reduce the number of preamplifiers employs a network of external resistors, arranged as
a series of resistive dividers, to identify the activated strip [Gerber 1976]. The top array of strips has two
preamplifiers, one each attached to outermost strips, connected consecutively to each inner strip through
a resistor division circuit. The difference or ratio of signals from each end is used to determine which of
the strips was activated by an event. The sum of the signals preserves the energy information. Employing
the same scheme on the backside orthogonal strip array, the two perpendicular strips closest to the ionizing
event can be identified. Gerber et al. [1977] manufactured these detectors as position sensitive gamma-ray
detectors, and, hence, they use Ge wafers instead of Si in order to increase the interaction probability. To
prevent cross conduction and isolate the strips from each other, the strips have trenches etched between
them.
Particle detectors employing the same external resistive divider scheme as Gerber et al. [1977] have been
fabricated with common Schottky barrier designs by applying Au strips and Al strips on opposite sides of a
ν-type Si wafer [Lamport et al. 1976, 1981; Heijne et al. 1980]. Position resolution of 150 μm was achieved
for energy deposits of 60 MeV from 60 Fe ions. To reduce leakage currents between adjacent strips, it is
common to use SiO2 insulation between the strips. This oxide is grown through high-temperature methods,
and photolithography is used to pattern and define the locations of the microstrips. The oxide is etched back
730 Semiconductor Detectors Chap. 16

+
Figure 16.15. (left) For a space charge density of ND = 3.33 × 1011 cm−3 , the calculated voltage
distribution for a section of a 150 μm wide pixellated diode with 50 μm × 50 μm pixels. (right) The
resulting weighting potential for a single pixel of the same device.

to the bare Si to which the strips are to be applied. Implantation or traditional dopant diffusion is used
to apply the p and n contacts, over which metal is applied, producing the end result shown in Fig. 16.14.
However, Lutz [1999] points out that the oxide may be a cause of eventual device failure unless critical
design features are not in place. Silicon dioxide can have residual impurity ions (such as Na+ ) or may incur
radiation damage that produces positive space charge. This space charge attracts electrons at the oxide-
silicon interface and can form a conduction path between the strips, consequently, shorting adjacent strips.
Proposed solutions to the problem include p-type implantation between the strips and producing negatively
biased MOS structure atop the oxide strips [Lutz 1999].

Pixellated Detectors Spatial resolution can be improved by simply placing an array of contacts on a
semiconductor surface and connecting each contact to a separate output. These contacts are referred to
as pixels (or sometimes pads) and this detector structure has several advantages, which include increased
energy resolution from the asymmetric weighting potential, reduced capacitance of each pixel, reduced leakage
current flowing to each pixel, and relatively fast response times.
Shown in Fig. 16.15 are the calculated operating and weighting potentials for a pνn pixel detector
fabricated on high-resistivity Si (ND +
= 3.3 × 1011 ). The back plane of the design is a p-type contact
fabricated on a ν-type substrate, with n-type anode ohmic contacts. The voltage distribution is nearly the
same as a planar detector, indicating that charge carriers are collected as expected from a common planar
device. However, the weighting potential for each pixel is highly non-linear with most of the induced current
appearing on the output as free charges drift in the near-anode region. This effect is commonly referred to as
“the small pixel effect,” and was initially explored by Barrett et al. [1995] (see also Eskin et al. [1995]). If the
pixel size is smaller than the final charge carrier cloud size, largely affected by the initial ionizing event and
the charge carrier diffusion thereafter, then more than one pixel is expected to sense the arrival of electrons.
This problem is denoted as “pixel-sharing” and leads to confusion about where the initial event occurred in
the detector. This effect is reduced by increasing the pixel size, but at the expense of spatial resolution.
The capacitance of a pixel strongly affects the electronic noise and ultimately the potential developed by
the induced charge. A single square pixel has an area of n2 , where n represents a side dimension, so that a
microstrip of length L has an area of n × L. The expected increase in capacitance for the microstrip is L/n;
hence, the output voltage for the microstrip decreases by a similar amount for the same induced charge. The
Sec. 16.4. Detectors Based on Group IV Materials 731

lower leakage current produced by a single pixel also reduces the electronic noise sensed by the preamplifier
circuit. Mouthuy [2005] reports on comparisons of various pixel detectors for high energy physics applications
with the claim that some pixel devices can have 15× lower electronic noise than microstrip counterparts.
Consequently, because of the lower signal-to-noise ratio, thinner detectors can be used while still discerning
events from noise, even with the reduction in energy deposition. Finally, because of the asymmetric charge
induction from the small pixel effect, most of the charge induction appears on the output within 10 ns,
thereby improving timing resolution of events.
However, there are complications with high-density pixel detectors. The pixel detector design requires as
many readouts as detector contacts, a requirement that can be very demanding on the readout electronics.
As pixel resolution increases, the readout density also must increase and can be cumbersome for traditional
wire bonding methods. Instead, it is common to bond the pixel detector to an application specific integrated
circuit (ASIC) designed as a miniaturized preamplifier readout for a high-density array of detectors. The
detector contacts are connected to the readout electronics by a “flip-chip” method, originally developed by
General Electric [1963]. This method permits the face of the pixel device to be aligned directly atop a
readout microchip. The contact pads of the microchip have solder patterned on each contact. When heated,
the solder forms into a ball from its own surface tension, and is afterwards allowed to cool. Hence, the ASIC
chip has an array of soft solder balls exactly placed at the locations of the detector pixels and the readout
contacts. The detector is pressed onto the soft solder, commonly an indium alloy, and heated to solder the
two parts together [Broennimann et al. 2006]. Indium solder is commonly used because the different alloys
have low melting points, ranging from 7◦ C to 310◦ C. Under some conditions, the mechanical compression of
the lower temperature alloys is adequate to form a bond, thereby removing the heating requirement [Lozano
et al. 2001]. Indium is also malleable and less prone to fracture under stress or from thermal expansion
mismatch.

Drift Diode Detectors Large area planar detectors can have significant capacitance that reduces pulse
height and increases detector electronic noise. Consequently, surface barrier detectors and the like are usually
limited to modest diameters, with most commercial units having less than 40 mm diameter, although there
are some special-application implanted-junction detectors with up to 60 mm diameter active regions. This
problem of increased capacitance is largely mitigated with the drift diode design, a clever device that has
a small anode with numerous guiding electrodes, invented by Gatti and Rehak in 1984 (see also Gatti et
al. 1985). There are several variants on the design, the most common are the linear drift diode and the
concentric ring drift diode [Lutz 1999].
The linear drift diode design concept is shown is Fig. 16.16, having a high purity substrate with multiple
reverse biased pn junction strips aligned parallel on the front and back surfaces. One or more collection
electrodes are established on one side, usually at one end of the strip array or near the center of the device
between several microstrips. Because electrons have higher mobility in Si, it is usual to fabricate the device
from ν-type material with p-type cathode strips on the surfaces. The collection electrode(s) is an n-type
ohmic contact and is the location of the output electronics.
The device is operated under reverse bias, with gradually increasing positive voltage applied to each drift
field electrode from the outermost strips towards the collection anode. This potential distribution can be
accomplished by employing a resistive divider along the distribution of microstrips. At full depletion, from
both sides of the substrate, the residual space charge forms a potential valley near the center of the volume
as shown on the left of Fig. 16.17. It is interesting to note that the potential valley does not form without
the benefit of some space charge (ND +
or NA− ) being present. Ionizing events that occur in the device produce
electron-hole pairs. Electrons drift to the bottom of this potential valley and are guided to the anode. The
resultant weighting potential of the configuration causes most of the induced charge to be sensed as the
electrons transit past the last drift electrodes and to the anode (see Fig. 16.17 (right)).
732 Semiconductor Detectors Chap. 16

Vc Vc - 4Dv
R R R R R R R
cathodes
d es
a no

oxide
+
- - ++
n-type - -
contact - - - - - - ++ ++ p-type junctions
- - + +
n-type Si +
- - ++ +
+
oxide
cathodes

Figure 16.16. Structure of a linear Si drift diode detector. After excitation,


electrons are drifted through a central potential channel and collected at an anode.
Holes are collected at nearby cathodes. The output signal is heavily weighted on
the electron induced charge as they near the anodes. After Gramegna et al. [1995].

+
Figure 16.17. (left) For a space charge density of ND = 1012 cm−3 , the calculated voltage distribution
for a 150 μm wide linear Si drift diode near the anode region. (right) The resulting weighting potential
for the same device.

A drift detector design employing ν-type Si material with a series of p+ contact concentric rings is
described by Gatti et al. [1985] and Lechner et al. [1993; 1996]. The device can be larger than the linear
design but still have the advantage of low capacitance. Lechner et al. [1993; 1996] include a first stage field
effect transistor (FET) input on the detector, which further reduces capacitance and electronic noise. The
detector anode is near the center, but actually surrounds the output FET. The design has another difference
from the basic linear design first proposed by Gatti et al. [1984a, 1984b], in that the drift field electrodes
are only on one side of the device. The backside of the detector is a simple p+ planar contact, used to
promote full depletion of the device. Performance for a 300 μm thick concentric drift diode of 3.5 mm2 area
yielded room-temperature (300 K) FWHM energy resolution of 220 eV for 5.9 keV photon emissions from
55
Fe. When cooled to 150 K with a thermoelectric cooler (Peltier cooler), the energy resolution reduced to
Sec. 16.4. Detectors Based on Group IV Materials 733

p p
n n
p p
n n
p p
n n semiconductor
substrate
n p
Figure 16.18. (left) Isometric view of the basic 3D architecture, showing interspersed n and p columnar
dopant columns in a semiconductor substrate. (right) Top view of a few proposed 3D patterns.

139 eV at FWHM. Lechner et al. [1996] also describe an array of drift diodes on a single substrate that can
be read out individually for position sensing information.
There are several advantages to the drift diode design. First, the device design (linear, concentric ring, or
variant) allows the realization of a relatively large area device with significantly reduced capacitance compared
to a planar device of the same area. Second, these detectors can be fabricated by common VLSI processing
techniques, thereby enabling mass production. Finally, drift diode detectors can be used as direct conversion
devices for x rays or can be used as light sensitive photodetectors for scintillation detectors, especially for
scintillators with longer wavelength emissions which are usually mismatched for bi-alkali photomultiplier
tubes. Avset et al. [1991] note that non-uniformities with material resistivities and charge carrier diffusion
broadening can adversely affect drift times and position information for two-dimensional readout schemes.
They further conclude that best results are obtained with drift fields that exceed 100 V cm−1 .

Silicon Three-Dimensional (3D) Detectors Radiation detectors at the Large Hadron Collider (LHC) re-
ceive over 1015 n[1MeV]eq cm−2 ,12 an indication that these detectors must survive this excessive dose. With
upgrades to a high-luminosity LHC, this fluence is expected to exceed 1016 n[1MeV]eq cm−2 [Bates et al. 2011].
Introduced in 1997 by Parker et al., three-dimensional detectors offer an alternative architecture for radiation
hardened particle physics detectors than do microstrip or pixel designs. These detectors are constructed as
vertically oriented pin diodes penetrating deep into a semiconductor substrate (see Fig. 16.18).
There are two salient advantages to the 3D design. First, the short distance between electrodes tremen-
dously reduces the collection time, thereby countering the expected reduction in τ ∗ and λ∗ for electrons and
holes after extreme neutron damage. The recoil damage to the crystalline structure increases with fast neu-
tron fluence, and consequently, the charge carrier trap density also increases. This increase in trap density
causes a reduction of the electron and hole mean free drift times. Unfortunately, it has been documented
that irradiation of 1016 n[1MeV]eq cm−2 for a Si detector reduces the electron and hole mean free drift times
τ ∗ to 0.24 ns and 0.16 ns, respectively [Bates et al. 2011]. These low values of τ ∗ correspond to mean free
drift lengths λ∗ of only 24 μm for electrons and 16 μm for holes. Recall from Sec. 15.4.6 the advantage of
increasing the carrier extraction factors  = vτ /W for electrons and holes leads to improved charge collec-
tion. The value of e,h can be increased by reducing the drift distance W between the detector contacts,
accomplished with the 3D design by producing adjacent penetrating contacts only tens of microns apart.
The resulting induced charge output ΔQ does not suffer as badly for the 3D design as compared to the signal
produced for charges drifting across the substrate width of a planar detector. Second, the capacitance of the
small electrodes is lower than a planar detector of the same total mass (thickness). Hence, the electronic

12 The compound unit “n[1MeV]eq cm−2 ” describes the equivalent dose damage per square centimeter fluence from a radiation
source as expected if the detector were irradiated with monoenergetic neutrons of 1 MeV energy.
734 Semiconductor Detectors Chap. 16

noise level should be reduced compared to a planar design, thereby enabling the observation of small pulses.
Together these advantages yield particle detectors capable of withstanding high doses of neutron damage.
The first designs had alternating offset rows of p+ and n+ holes etched into a 300 to 600 micron thick
Si substrate. These holes had diameters of about 15 to 30 microns [Kenney et al. 1999]; later designs had
smaller holes down to 10 microns in diameter [Da Viá et al. 2008; Pellegrini et al. 2008]. The holes are
etched deep into the substrate, sometimes completely through, with depths usually ranging between 250 to
300 microns. The pitch between adjacent holes is varied, but can be as low as 30 microns [Pellegrini et al.
2008].
The original 3D detectors were fabricated on one surface of a Si semiconductor substrate and are often
referred to as “full 3D detectors” [Bates et al. 2011]. Da Viá et al. [2008] comment that p-type wafers are
probably a better choice for the detector substrate and apparently are not susceptible to type-inversion.13
The penetrating holes were etched with inductively coupled plasma reactive ion etching (ICP-RIE) methods
[Kenney et al. 1999]. To provide additional mechanical strength during the fabrication process, these first
devices were bonded to a Si support wafer. An array of holes was etched and doped p+ , followed by a backfill
of polysilicon to produce a relatively flat surface for the next process steps. A second array of holes was
then patterned between the first array, etched, and doped n+ . This second array of holes was also backfilled
with polysilicon. The final steps included patterning conductive leads to the separate arrays, dicing the
detectors from the wafer, and removing the support substrate. To mitigate dead regions around the detector
perimeter, electrodes were later patterned around the edges of the detectors [Kenney et al. 2001, 2006]. Da
Viá et al. [2008] report that full 3D detectors retained 38% charge collection efficiency after irradiation of
6.8 × 1015 n[1MeV]eq cm−2 , equivalent to approximately 10 years of operation within the Super-LHC.
The double-sided 3D architecture was introduced to simplify
In bump
poly n+
the fabrication process while reducing cross contamination of the
passivation passivation p and n doped columns [Pelligrini et al. 2008; Zoboli et al. 2008].
metal metal metal The holes are etched from both sides of a semiconductor sub-
oxide oxide
strate, with one side doped p+ and the other side doped n+ .
p-Si
p-dopant p-dopant The holes are arranged in an interspersed pattern such that the
p+ and n+ columns are adjacent. The holes are etched blind
285 mm

such that they do not penetrate completely through the wafer


250 mm

(see Fig. 16.19). Bates et al. [2011] reports on Si 3D detectors


n-dopant
with dimensions shown in Fig. 16.19, and for which the detec-
oxide oxide tors continued to deliver 47% charge collection after irradiation
oxide equivalent damage of 1016 n1MeVeq cm−2 at 150 volt bias. At
poly p+
metal higher voltage, charge multiplication was observed from the de-
10 mm 10 mm
vice, indicating impact ionization gain. Additional experiments
55 mm
conducted with double-sided 3D detectors fabricated from both
Figure 16.19. Structure of a p-type Si double- p-type and n-type substrates continued to deliver up to 70%
sided 3D detector (not to scale). After Pelligrini charge collection efficiency at 2 × 1016 n[1MeV]eq cm−2 [Köhler et
et al. [2008] and Bates et al. [2011]. al. 2011]. The n-type detectors did not show type-inversion. Be-
cause of the straightforward fabrication process and the high radiation hardness, up to 25% of the insertable
B-Layer (IBL) Si detector ring has been populated with double-sided 3D detectors during a recent upgrade
[CERN 2010; Lange 2015].

Charged Coupled Devices (CCD) The charged coupled device, or CCD, is an imaging device used to
register the intensity of energy deposited as a function of position. When color filters are added to the

13 The reversal of a rectifying junction that occurs from radiation damage turning n-type silicon into p-type silicon.
Sec. 16.4. Detectors Based on Group IV Materials 735

V3
V2
metal
V1 oxide

VID VIG VOG VOD

depleted region
--- ---
transfer direction
n+ contact p+ contact
p+ contact n+ contact
p-type Si

t2 ID IG 1 2 3 1 2 3 OG OD
t1 t3 t6 t7 OUT
ID
t4 t1
IG t2
t5
1 t3
2 t4
3 t5
OUT t6
t7
Figure 16.20. Depiction of a MOS n-channel CCD and its operation. (top) A cross section
depiction of a surface channel CCD showing only six transfer registers. (left) The clock waveforms
and output signal. After Kim [1979].

system, the CCD is used for optical photography and video imaging. The history of the CCD extends back
to 1970, when the inventors Boyle and Smith first described its function and operation. The first report on
an operating device was also published in 1970 [see Amelio et al. 1970]. This first device was designed as
a series of metal pads placed atop a SiO2 layer grown on a n-type Si substrate to produce a series of MOS
capacitors in line on a substrate. Although these first-generation devices had multiple problems with charge
sharing and incomplete charge transfer, modern optical devices are still based on improved MOS designs.
Damerell et al. [1981, 1987, 1990] and Bailey et al. [1983] report the use of MOS CCDs for radiation detection
applications. Advantages of the CCD concept include a reduced number of readout electronics for the large
number of pixels, small pixel sizes for good spatial resolution, and relatively rapid response [Stefanov 2006].
Further, CCDs can be tiled to produce a much larger detector array.
The general operation of the CCD is often described with a simple MOS structure as an example, such as
the 3-phase surface-channel MOS CCD depicted in Fig. 16.20. The device of Fig. 16.20 has a series of MOS
diodes fabricated on a continuous surface of SiO2 . At the ends of the MOS diodes are input and output
structures that consist of an input diode and gate (ID and IG) and is used to inject charge and an output
diode and gate (OD and OG) that is used to collect charge [Sze 1981]. Because the charge to be measured
is excited by radiation events in the depletion region, charge injection is not a necessary requirement for
radiation detection CCDs but is used here to provide an example of the charge transport. Every third gate
contact, or transfer register, is biased at the same potential, labeled V1 , V2 , and V3 . The transfer registers
can be fabricated as strips, and the orthogonal crossing of each register strip along the transverse direction
736 Semiconductor Detectors Chap. 16

constitutes a pixel. A digital clock is used to time and apply voltages to the gates in a sequential order. The
voltages applied at the input and output diodes are biased high enough to produce deep depletion regions
underneath the input and output gates. At time t1 , the voltage applied to V1 is higher than V2 and V3
and produces deeper depletion wells at all positions 1. At t2 , the voltage is adjusted to reduce the barrier
between ID and V1 , which allows charge to flow into the first well. At t3 , VID is increased to close the gate,
while excess charge is removed through the ID contact. A t4 , V1 is lowered and V2 is increased, causing
the depletion wells at 1 to decrease and depletion wells at 2 to increase. Consequently, charge flows from
positions 1 into positions 2, a process named charge transfer. This process is continued, as depicted for t5
through t7 , until the charge is transferred to the output diode. The process is often described as analogous
to a ‘bucket brigade’. A similar shift register, oriented orthogonal to the CCD gate transfer registers, can be
used to read the output from each row of transfer registers. There are many variations of MOS CCDs, and
Fig. 16.20 depicts only one of many [Kim 2009; Sze 1981; Schroder 1990; Lutz 1999]. Each entire readout of
the CCD array is called a ‘frame’ and the pixels are often termed ‘gates’. Each row of registers is read out
such that the synchronized clocking electronics can identify the pixel origin when the charge appears on the
output.
Recall the description of MOS devices given in Sec. 15.3.4, where again the terms for flat band voltage
VF B and gate voltage VG are used here. The surface potential ψs under a CCD gate is defined as

qe N A W 2
VG − VF B = Vi + ψs = + ψs , (16.28)
Co
where W is the depletion layer width, NA is the semiconductor doping concentration, Co is the oxide layer
capacitance in F cm−2 , Vi is the potential drop across the insulating oxide layer, and

qe N A W 2
ψs = , (16.29)
2κs 0
where κs is the dielectric constant for the semiconductor. Rearrangement and substitution of the definition
of W into Eq. (16.28) gives
1
VG − VF B = ψs + [2κs 0 qe NA ψs ]1/2 . (16.30)
Co
As charge is accumulated in the potential well under the gate, the gate voltage is altered to become

Qs [2κs 0 qe NA ψs ]1/2
VG − VF B = + + ψs . (16.31)
Co Co
Solving this equation for ψs gives
  1/2
Qs Qs
ψs = VG − VF B + V0 + − 2 VG − VF B + V0 + V02 , (16.32)
Co Co

where Qs is the stored charge per unit surface area and


qe N A κ s  0
V0 = . (16.33)
Co2

The maximum charge that can be stored in a single pixel is described by [Schroder 1984] as

Qmax = −Co (VG − VF B − 2ψB − VB ) , (16.34)


Sec. 16.4. Detectors Based on Group IV Materials 737

where   1/2
kT NA 4qe κs 0 NA ψB
ψB = ln and VB = . (16.35)
qe ni Co2
Under the assumption that both VB and ψB are small by comparison to the applied effective operating
voltage VG − VF B , Eq. (16.34) becomes

Qmax ≈ −Co (VG − VF B ) . (16.36)

The gate oxide is typically about 100 to 200 nm thick and the difference in gate voltage is usually 5 to 10
V. Pixel dimensions for scientific CCDs can range from 50 microns down to 1 micron, and CCDs can have
over 2 megapixels in a single device. Commercial CCDs for x-ray imaging applications typically have 20 ×
20 micron pixels. If the charge accumulated in a potential well exceeds the capacity, then mobile charges
can diffuse into adjacent pixel wells, causing a blurring or a washed out line to appear in the image.14 A
typical charge limit for a MOS CCD potential well is about 5 × 106 electrons [Schroder 1990].

Example 16.2: A common surface channel MOS CCD has pixel sizes of 20 × 20 microns. The oxide
thickness is 0.2 microns and the effective operating voltage is 10 volts. Determine the maximum charge that
can be stored under the gate.

Solution:
The capacitance per unit area Co is

κo 0 (3.9)(8.854 × 10−14 F cm−1


Co = = = 1.73 × 10−8 F cm−2
Wo 2 × 10−5 cm
The maximum charge capacity is

Qmax = −Co (VG − VT ) = (1.73 × 10−8 F cm−2 )(10 V)(2 × 10−3 cm)2 = 6.9 × 10−13 C.

This charge corresponds to

6.9 × 10−13 C
number of electrons = = 4.3 × 106 electrons.
1.6 × 10−19 C/e−

The surface n-channel device has some problems with efficient charge transfer from one gate register
to an adjacent register, mainly because the lowest part of the potential well is adjacent to the oxide layer.
To improve transport efficiency, the buried n-channel CCD, or BCCD, was introduced, in which an n-type
tub is deep diffused into the p-type bulk, upon which the oxide is grown [Walden et al. 1972]. The BCCD
architecture moves the lower point of the potential well away from the surface and into the semiconductor
bulk [Schroder 1990].
MOS-based devices can have many problems when used as radiation detectors. First, the oxide can be
destroyed by ionizing radiation by producing stationary trapped charge, ultimately changing the operating
voltage of individual pixels and causing failure [Killiany et al. 1974, 1975, 1980]. Further, common small pixel
CCDs do not have the capacity to store charge for high-energy particles, such as alpha particles, causing
charge overflow into adjacent pixels. Finally, the pixel sizes are usually small with depletion region depths

14 You may have seen this effect when pointing your CCD camera at a candle or other bright light.
738 Semiconductor Detectors Chap. 16

V1
V2 V+
oxide n+ collecting
V3 contact

p+ contacts --- ---


minimum of potential
depleted transfer direction valley for e- transfer
(from pixels) depleted
n-type Si
(from back)

p+ back contact
V-
Figure 16.21. Fully depleted pn junction type CCD, depicting a cross section
portion. After Strüder et al. [1987a, 1990].

of about 1 to 3 μm [Lutz 1999], and energetic particles deposit only a small portion of energy in a single
pixel. In some cases, a particle can transit across many pixels.
The pn-junction design, proposed by Gatti and Rehak [1984a, 1984b], has received interest as an al-
ternative for radiation imaging applications. A cross section of this device is depicted in Fig. 16.21. The
pn-junction CCD has three operating voltages synchronized by a clocking circuit [Strüder et al. 1987b, 1990].
The device is reverse biased from an n-type contact against a p-type back contact and the multiple p-type
pixel contacts, resulting in a fully depleted ν-type Si substrate. A pixel is defined by the orthogonal crossing
of a p-type strip transfer register with that of a n-type channel guide (see Strüder et al. 1987b). The three
operating voltages (V1 , V2 , V3 ) are altered to move the potential minimum along the length of register pixel
contacts towards the anode. As these voltages are changed, the lowest potential is moved along the contacts
towards the anode, ultimately forcing charges to sequentially move from the region under one contact to an
adjacent contact. The design is improved by adding channel guides in the direction of motion towards the
anode and are composed of an implanted n-type region perpendicular to the p-type transfer pixels [Strüder
et al. 1987a]. These channel guides prevent punchthrough currents between the p-type contacts. They also
provide a route for the moving charges and reduce lateral diffusion of charges to pixel locations at the sides.
There are additional advantages of the fully depleted pn-junction CCD. Because the entire volume is
depleted, the pn-junction CCD has a large active region, leading to enhanced efficiency over the MOS type.
Further, a relatively thin backside p-type contact allows the device to be operated with the backside under
illumination, thereby producing a much more uniform response of the device area. Because the volume
is depleted from top and bottom, the potential minimum is displaced from the surface, unlike that in a
traditional MOS CCD, and the charges can travel much faster through the device to the anode. The pn
junction is more radiation hard than the MOS version; hence the pn-junction CCD is more suited for
operation in a radiation environment.
There are two common methods by which CCDs function for radiation imaging: (1) as optical detectors
for scintillating materials and (2) as direct conversion detectors. Scintillators can be attached to a CCD and
the light response spatially measured by the CCD. Methods include the direct attachment of scintillating
material to the CCD, although this method puts the CCD in the radiation field. Resolution can be enhanced
by having the CCD displaced from a large scintillating screen with the image focused and projected onto
the CCD, often with mirrors or a light waveguide [Gruner et al. 2002]. Thick scintillators increase efficiency,
but also cause a reduction in spatial resolution. Phosphor-coated screens preserve the spatial resolution,
but often have reduced efficiency for high-energy particles. However, for low energy particles and x rays,
phosphor screens can provide a suitable detection medium. In a study comparing phosphor screens for x-ray
computed tomography, having either lens-coupled CCDs and fiber-coupled CCDs, the lens method provided
higher spatial resolution [Uesugi et al. 2011]. However, the light transmission of the fiber-coupled system
Sec. 16.4. Detectors Based on Group IV Materials 739

was four times more efficient than the lens-coupled device. Consequently, the higher transmission efficiency
enables a fourfold reduction in the exposure time. Further, samples prone to deformation are less affected by
the reduced exposure time. Finally, the radiation dose to patients is lower because of the shorter exposure
time.
The direct imaging method relies on ionizing radiation producing electron-hole pairs in the depleted
sensitive region of the CCD. The obvious problem with this approach is that the CCD is placed in the
radiation field, and defect formation can eventually cause device failure. This failure is especially problematic
when irradiated with heavy ions and reaction products emitted from neutron conversion films. Regardless,
the direct conversion method has been used for detection of MIPs in Vertex detectors for high energy physics
applications [Damerell 1998, 2003, 2005; Turala 2005; Stefanov 2006; Ishikawa 2015]. Direct conversion CCDs
can be commercially acquired for x-ray imaging applications [Hammamatsu 2016]. Windowless CCDs are
front irradiated and are designed to detect x-ray energies between 0.5 keV and 10 keV. The back irradiated
versions are designed with a thinned surface layer to detect lower energy x rays and also have thicker depletion
regions for higher x-ray energies.
For low energy photons, CCDs can be used as photon counters and direct conversion spectrometers.
However, charge sharing between pixels can degrade energy resolution and confuse the photon counting,
especially for surface channel and BCCD MOS devices in which a large portion of the semiconductor is not
depleted. Photon interactions can cause ionization in the undepleted portion, and through charge diffusion,
electrons can be shared with many pixels [Lumb and Nousek 1992]. To reduce this problem, CCDs operated
as photon counters should have no more than approximately 0.15 photons per pixel per frame to stay within
1% count error. Photon spectroscopy is even more demanding, reportedly requiring about 0.018 photons
per pixel per frame [Lumb and Nousek 1992]. The chance of additional interactions during charge transfer
process increases with increasing radiation fields, and may pose a problem if radiation spectroscopy is the
desired outcome [Lumb and Nousek 1992], mainly because the total background events per frame increases.
The clock sampling rate can be increased, but unfortunately this change also causes the signal to noise ratio
to decrease. To reduce background charges during the readout process, Lumb and Nousek [1992] also suggest
the implementation of a shutter during readout.
As with all semiconductors, leakage current has a generation-recombination component. Hence, CCDs
operated at room temperature thermally generate electron-hole pairs during operation and during charge
transfer. Usually room temperature operation does not pose a problem. However, for low light or low
radiation environments, thermal noise can cause image degradation. This problem is remedied by cooling
the CCD during operation between 173 K to 223 K.

Si(Li) X-ray Detectors


The low Z number and low volume density of electrons causes the γ-ray absorption coefficient to be small
for Si. Further, the energy at which the photoelectric absorption and the Compton scattering are equal is
relatively low at only 60 keV. The Compton scattering coefficient is much lower than most semiconductors
used for radiation detection (see Fig. 16.1). Hence, Si is a poor choice for high energy γ-ray spectroscopy.
However, its K absorption edge appears at 1.838 keV, meaning that the absorption edge discontinuity does
not adversely affect x-ray absorption at higher energies, nor does the appearance of x-ray escape peaks cause
significant issues in spectra. By comparison, the K absorption edge for Ge is 11.103 keV. Because higher
energy γ rays have less chance of interacting in Si, this property serves to reduce background effects. For
these reasons, Si does have importance as an x-ray spectrometer for applications such as x-ray fluorescence,
x-ray microanalysis, particle induced x-ray emission (PIXE), x-ray absorption spectroscopy (XAS), x-ray
diffraction, and Mössbauer spectroscopy at energies generally below 50 keV. Energy resolution is the full
width at half the maximum (FWHM) of a spectral full energy peak. Silicon detectors deliver excellent energy
740 Semiconductor Detectors Chap. 16

resolution, and the FWHM, reported in units of energy, is

FWHMeh = 2 2 ln(2)wEγ F , (16.37)

where w is the average energy to produce an electron-hole pair, Eγ is the photon energy, and F is the Fano
factor (typically 0.12). The Fano factor is a correction factor that accounts for the typically higher energy
resolution than predicted from pure Gaussian statistics. With the inclusion of noise sources, the energy
resolution becomes   1/2
FWHM = (FWHMnoise )2 + (FWHMeh )2 . (16.38)
where the FWHMnoise contribution includes electronic noise and fluctuations in the leakage current.
Highly purified Si can be fashioned into a type of pn, pπn, or pνn diode; yet, even with zone-refined high-
purity material, Eq. (15.61) (or Fig. 16.11) show these devices are limited to depleted regions less than 2-mm
wide, an unsatisfactory thickness for efficient x-ray absorption. The problem is remedied by compensating the
remaining impurities in Si with the Li-drifting technique. Pell [1960b] introduced the process of Li drifting
in Si, a method to electrically drive Li+ ions deep into a semiconductor, in which Li behaves as an n-type
dopant. If the Si material is π-type, these Li+ ions exactly compensate the negative space charge effects of
acceptor impurities and, thus, the Si material behaves as if it were intrinsic-like. Although other Group I
alkali metals such as Na and K also act as donor impurities in Si, it is the small atomic radius and high
interstitial drift mobility of Li that makes the drift process possible [Pell 1960b]. Unlike common impurity
dopants such as B, P, and As that become electrically active by displacing Si atoms in the crystalline lattice,
Li ions become interstitial donors lodged between lattice sites with an ionization energy of 0.03 eV [Mann
et al. [1962].
Li drifting is fundamentally a three-step process, starting with producing a pn junction diode, into
which Li is introduced as the n-type dopant onto a p-type slab. A purified single crystal of p-type or π-
type Si sample is sliced and etched to appropriate dimensions. Afterwards, Li is applied to the surface of
the Si slab. There are many processes to apply Li to the Si surface, including physical vapor deposition
[Blankenship and Borkowski 1962; Mann et al. 1962; Ristenen et al. 1967] and application of a suspension
of Li in oil [Ammerlaan and Mulder 1963; Mayer 1962]. Painting the Li-oil suspension on the sample
seems straightforward; however, if done improperly, the layer can be uneven and form cracks, consequently
producing a uneven Si surface once the diffusion process is finished. The Si sample is then heated to
approximately 400◦C for several hours. This Li predeposition process produces a pn junction at the surfaces
in contact with the Li dopant. The Li distribution after this predeposition step is
 
x
ND (x) = N0 erfc  , (16.39)
4Dtp
where N0 is the initial donor concentration, D is the diffusion coefficient, and tp is the process time. Pell
[1960a] measured the diffusion of Li in Si at temperatures between 25◦ C and 125◦C. Combined with data
acquired elsewhere [Fuller and Severiens 1954], Pell [1960a] estimates the diffusion coefficient dependence
as15
−qe (0.655 ± 0.01)
D(T ) = (25 ± 2) × 10−4 exp cm2 /s, (16.40)
kT

15 Based on the data from Fuller and Severiens [1954], the Li+ ion mobility as a function of temperature can be estimated with
the result of a least squares fit
−7733.45
D(T ) = 28.91 × 10−4 exp cm2 /s.
T
Although this result differs from that reported by Fuller and Severiens [1954], it is similar to that found by Pell [1960a].
Sec. 16.4. Detectors Based on Group IV Materials 741

where T is the absolute temperature in Kelvin. After the Li deposition step, Pell [1960b] approximates the
Li distribution by expanding Eq. (16.39) as

2N0 Dtp −x2
ND (x)  √ exp . (16.41)
x π 4Dtp

Because NA = ND at location c in Fig. 16.22



2N0 Dtp −c2
NA  √ exp , (16.42)
c π 4Dtp

so that 
c π c2
N0  NA exp . (16.43)
2 Dtp 4Dtp
Upon substitution of Eq. (16.43) into Eq. (16.41) one finds

c c2 − x2
ND (x)  NA exp . (16.44)
x 4Dtp

Afterwards, the temperature is lowered, usually be-


tween 100-200◦C, and a reverse bias is applied to the
diode [Ammerlaan and Mulder 1963; Miller et al. 1963]. N0 ND
This primary drift serves to force the Li+ ions deep into

log of concentration
ND
log of concentration
surface

the Si material and enlarge the compensated thickness.


NA NA
Miller et al. [1963] point out that the thermally gen-
erated charge carrier density (and reverse leakage cur-
rent) increase with drift temperature. At too high a
W
drift temperature, the thermally generated electron and
hole concentrations can exceed the donor space charge
concentration. Consequently, the compensation process c x a c b x
can become non-uniform and incomplete. Goulding and Figure 16.22. The impurity concentrations for Li (ND )
Hansen [1964] point out the importance of temperature and the acceptors (NA ) (left) directly after the Li diffusion
and current control over the process to maintain good process and (right) after the ion drift process. W represents
compensation uniformity. Periodically during the drift- the compensated region.
ing process, it is possible to stop the drift and measure the reverse current and capacitance to yield a measure
of the compensation region width [Ammerlaan and Mulder 1963; Dearnaley and Lewis 1964], mainly because
capacitance is inversely proportional to the width while the generation current is proportional to the width.
For the general analysis of the Li+ ion drift, it is assumed that the distribution of acceptor impurities
NA is uniform and constant. The Li+ ion mobility in Si can be described by [Blankenship and Borkowski
1962]  
1000 1000
μLi (T ) = 2.78 × 10−2 exp −7.5 , (16.45)
T T
where T is the absolute temperature in Kelvin. Assuming that the drift force μLi END is much greater
than the diffusion force D∇ND , the initial Li+ concentration at locations x < c decreases and the Li+
concentration at locations x > c increases. As the compensated region expands, the Li+ concentration at
x < a continues to decrease while the Li+ concentration at x > b continues to increase. Note that the Li+
concentration does not reduce below NA for x < c and does not exceed NA for x > c. If it could, then
742 Semiconductor Detectors Chap. 16

the space charge polarity would reverse in either region, causing Li+ to drift towards the negative space
charge until compensation was complete. The number of Li+ ions per cm2 , the ion current density, moving
across the junction boundary in time t is EμLi NA t and it is assumed the electric field is primarily in the
compensated region where ND  NA . Overall, the total number of Li+ ions drifted is represented by the
gray areas in Fig. 16.22. Near t = 0 at the beginning of the drift process, when W  2Dtp /c, Pell [1960b]
approximates the amount of Li drifted over time t as
 t  c  b
μLi ENA dt = ND (x) dx − (c − a)NA = (b − c)NA − ND (x) dx. (16.46)
0 a c

Insertion of Eq. (16.39) into Eq. (16.46) and use of



1
erfc(az) dz = z erfc(az) − √ exp(−a2 z 2 ), (16.47)
a π
which is obtained by integration by parts, yields
   
t c
c
μLi ENA dt = ND (x) dx − (c − a)NA = −(c − a)NA + cN0 erfc 
0 a 4Dtp
     
a N0  −a2 −c2
−aN0 erfc  + 4Dtp exp − exp . (16.48)
4Dtp π 4Dtp 4Dtp

A similar expression can be obtained in terms of a and c using the right-hand side of Eq. (16.46). A Taylor
expansion of the erfc and exponential functions in Eq. (16.48) about c gives

(c − a)2 (c − a)3
μEdt  + , (16.49)
2L 6L2
where L = 2Dtp /c. Pell [1960b] assumed that the compensated width W = (b − a)  L if tp is very small.
If the slope of the Li concentration is assumed linear at point c in Fig. 16.22, then at tp ≈ 0 the distance
c − a ≈ b − c, such that the first expansion term of Eq. (16.49) yields

W2
μLi Edt  . (16.50)
8L
As the drift process continues, it can be assumed that (b − c) (c − a) and W  (b − c), so that [Goulding
1966]
dW  μLi Edt. (16.51)
For a planar device where E = V /W , the solution for the compensated detector width is

W = 2μLi V t. (16.52)

By using both Eq. (16.45) and Eq. (16.52), Blankenship and Borowski [1962] develop a plot predicting the
compensated width of a planar Si(Li) detector as a function of temperature, time, mobility, and voltage.
The resulting devices usually have active regions with thicknesses between 3 and 5 mm; however, thicker
widths are possible [Ristinen et al. 1967; Bertolini and Coche 1968]. Sharma and Divatia [1986] report a
table of drift time and temperature that indicates a 5-mm compensated region takes 280 kilovolt hours at
110◦ C while raising the temperature to 130◦ C reduces the drifting duration to 115 kilovolt hours. Adequate
Sec. 16.4. Detectors Based on Group IV Materials 743

detail of a few drift procedures are provided in the literature [Blankenship and Borkowski 1962; Goulding
1965, 1966; Sharma and Divatia 1986].
The performance of Si(Li) detectors can be affected by detector volume and the initial distribution of
background impurities. Although the analysis performed above is a common treatment for the Li drift
process, there are many non-ideal situations that affect the outcome. Gibbons and Iredale [1967] and Lauber
[1969] analyze numerous alternative solutions that include nonuniform distribution of acceptors, the affect of
free charge carries, generation and recombination current, and the effect of trapping and detrapping on the
drift process. Gibbons and Iredale [1967] also analyze the expected Li drift result for a detector with coaxial
geometry. Contaminants in the Si can also cause problems with the process, further evidence that it is best
to start with relatively pure Si material. Pell [1961] and Ammerlaan and Mulder [1963] report that oxygen
contamination in the Si can adversely affect the drift process and drastically lower the Li+ ion mobility from
the formation of LiO+ -complex.
A second “clean up” drift at a lower temperature is usually performed after the primary drift process
[Lauber 1969], although this drift procedure is still conducted at a temperature higher than the detector
operating temperature. The second drift is conducted such that the thermally generated free charge carrier
density is much lower, thereby lowering the total space charge concentration. Sharma and Divatia [1986]
describe a “clean up” process in which the temperature is slowly reduced under bias as the drifting process
continues. Overall, the second drift process produces a much more uniform and complete compensation as
the Li+ ions redistribute.
Unfortunately, even with the second drift, there are usually some residual uncompensated centers, re-
sulting in a net space charge density [Gibbons and Ireland 1967]. These residual uncompensated defects
alter the electric field, pulse shape, and performance of the detector [Moszyński et al. 1968; Moszyński and
Przyborski 1968; Moroz and Moszyński 1969]. As explained in Sec. 15.3, space charge limits the depletion
thickness, and from Sec. 16.2.4, ionized impurities reduce the charge carrier mobilities. If the residual space
charge is uniform, then the electric field drops linearly, being lowest near the n-type contact. However, if
the residual space charge varies over the detector width, the electric field can have a much more complicated
distribution. The research of Mosziński and Przyborski [1968] indicates that the actual electric field dis-
tribution is parabolic in shape, a consequence of non-uniform compensation of the background impurities,
which appears to have a linearly varying distribution of space charge. The pulse shapes are dependent on
the radiation interaction location, and ultimately the operating voltage must be increased to sustain good
performance.
Llacer [1964, 1966] determined that the surface conditions and the junction geometry affect the perfor-
mance of a Si(Li) detector, noting that most of the surface current originates at the i-p junction where the
electric field is highest. Further, it was observed that an inversion layer can form on the periphery of the
Li-drifted region, where a n-type layer forms, thereby forming a junction around the device including atop
the p-type region. The consequence is low-breakdown voltage and relatively high surface leakage current,
both contributing to electronic noise. By changing the detector geometry, it was found that the surface
breakdown voltage could be increased and the leakage current decreased [Goulding 1965; Llacer 1966]. The
added advantage of a higher operating voltage is faster charge carrier collection times. Two popular Si(Li)
detector geometries used to increase surface breakdown voltage are depicted in Fig. 16.23, both pin-type
devices (discussed in Chap. 15). The inverted-T design includes a deeply etched trench surrounding the
n-type contact, while the etched planar design isolates the n-type contact away from the bulk p-type region.
Malm and Dinger [1976] and Goulding [1977] point out that the inverted-T design has regions with only
partial collection of charge carriers, mainly near the boundary of the etched trench where charges can be
collected at the trench. This charge becomes lost and consequently degrades the signal. An isolated guard
ring around the n-type contact isolates the detector sensitive region from the trench and improves overall
performance [Goulding 1977; Hau et al. 2003].
744 Semiconductor Detectors Chap. 16

n-type n-type
Au contact Au contact
region region

e
p e intrinsic p intrinsic
(Li-drifted region) h p (Li-drifted region) p
h

Schottky p-type p-type


contact dead layer Schottky dead layer
contact

Figure 16.23. Popular configurations for Si(Li) detectors, showing


(left) the inverted-T and (right) the etched planar.

Figure 16.24. The absorption efficiency of a Si(Li) detector as a


function of x-ray energy, depletion thickness, and entrance window.
Data from Canberra Industries, Inc. 2003.

Unlike the lithium-drifted version of Ge detectors, or Ge(Li) detectors, the Li+ ions remain locked into
position at room temperature. Although Si(Li) detectors can be operated at room temperature, they perform
best when cooled to low temperatures. Various Si(Li) detectors are available coupled to either liquid nitrogen
(LN2) dewars or Peltier coolers.
The detectors are encapsulated in a protective container with a thin entrance window, typically con-
structed from Be. The entrance window of the detector affects the low energy sensitivity limit. Shown
in Fig. 16.24 is the detection efficiency for various Si(Li) detectors with different thicknesses and different
entrance windows. Note that thicker detectors increase the efficiency for higher energy x rays, and an ap-
propriate choice of material for the entrance window can increase the detector efficiency for low-energy x
rays.
Si(Li) detectors are best used for spectroscopy of low-energy gamma and x rays. When cooled to cryogenic
temperatures (77 K), the resolution performance can be excellent. The energy resolution of a Si(Li) detector
can be predicted from Eq. (16.38), as shown in Fig. 16.25. An example x-ray spectrum from a chilled Si(Li)
detector is shown in Fig. 16.26.
Si(Li) detectors can be commercially acquired in a variety of segmented patterns, including strips, tri-
angular, and square patterns. The detectors consist of pin diode structures individually fabricated into a
Sec. 16.4. Detectors Based on Group IV Materials 745

Figure 16.25. The theoretical energy resolution of a Si(Li) detector,


which includes contributions from electronic noise. A Fano factor of
0.1 was used for the calculation. After Canberra Industries, Inc. 2003.

single Si substrate, thereby reducing “dead zones” between neighboring detectors. These detectors offer high
x-ray energy resolution and spatial interaction information. Further, clever designs can actually improve
count rate efficiency for ion probe instrumentation, such as PIXE, by surrounding the target region with
multiple detectors. Used in conjunction with other γ-ray detectors, the segmented Si(Li) detectors can be
used for Compton scatter γ-ray cameras. Properties of commercially available Si(Li) detectors are presented
in Table 16.6.

Table 16.6. Typical gamma-ray energy resolution of a few represen-


tative commercially available silicon semiconductor detectors. Many
other sizes are offered by the different vendors.
area energy FWHM
detector comments source*
(mm2 ) (keV) (keV)

Si(Li) 12.5 5.9 .155–.175 LN2 cooled C,O


5.9 .180
Si(Li) 20 Peltier cooled B
59.54 .450
Si(Li) 28–30 5.9 .165–.180 LN2 cooled C,O
Si(Li) 80 5.9 .175–.190 LN2 cooled C,O
Si(Li) 200 5.9 .220 LN2 cooled C,O
13 5.9 .18–.22
Si pin Peltier cooled A
25 5.9 .127–.230
∗A = AmpTek, B = Baltic Scientific, C = Canberra, O = Ortec.

Si(Li) β-Particle Detectors


At energies above 500 keV, the linear energy transfer (collisional) for fast electrons between 500 keV and 10
MeV is nearly constant (see Fig. 4.20). In Si the linear energy transfer ranges between 1.6 MeV cm2 g−1 (∼
3.8 MeV cm−1 ) at 500 keV to 1.92 cm2 g−1 (∼ 4.5 MeV cm−1 ) at 100 MeV. Unfortunately, excessive reverse
voltage is required to deplete surface barrier and pn junction Si diodes to thicknesses capable of recording
746 Semiconductor Detectors Chap. 16

Table 16.7. Maximum particle energy all of which is de-


posited in Si(Li) within a thickness x. Particles are nor-
mally incident on the detector and the thickness x is the
RCSDA (Emax ).
Thickness Electrons Protons α particles
(mm) Max Energy† Max Energy† Max Energy†
(keV) (MeV) (MeV)
0.1 116 3.19 12.5
0.2 177 4.75 19.0
0.5 321 8.13 32.5
0.8 444 10.7 42.6
1 522 12.1 48.4
2 889 18.0 71.8
5 1964 30.2 121∗
8 3085 39.4 157∗
10 3861 44.6 178∗

Figure 16.26. X-ray spectrum of a brass sample taken † Determined with the STAR series of codes [Berger 1992].
with a Si(Li) detector. ∗ Determined with TRIM 2013. See Zeigler et al. [2013].

meaningful energy deposition exceeding a few hundred keV. For instance, a surface barrier detector with
Nb  1012 cm−3 biased at -100 volts has a depletion region 250 microns wide, yet is capable of absorbing
the full energy of only about a 200 keV or lower energy electron (see also Table 16.7).16 This problem of
incomplete energy deposition is mitigated, somewhat, by using Si(Li) detectors, and indeed special planar
Si(Li) detectors are designed specifically for the purpose of energetic particle detection.
Detectors with active region depths between 4 mm to 8 mm are commercially available and are capable
of absorbing full electron energies ranging from 1.6 MeV to 3 MeV, respectively. Berger et al. [1969b] report
lower electron energy limits for some Si detectors, ranging between 20 to 40 keV, depending on the thickness
of dead layer which is the detector’s front contact. Here the 20 keV limit is for a surface barrier detector
and the 40 keV limit is for a Si(Li) detector. Should the detector width be less than the electron range,
then the electrons can pass completely through the detector and deposit only a fraction of their energy
[Berger et al. 1969a]. Consequently, a low energy tail, a consequence of partial energy deposition, forms in
the pulse height spectrum accompanied by a diminished full energy peak (as discussed further in Sec. 20.9).
Backscatter losses and bremsstrahlung energy losses can also add to the low energy tail [Frommhold et al.
1991]. Berger et al. [1969a] published tables of response functions that offer a method to determine the
energy deposition as a function of detector thickness. Modern Monte Carlo programs can also be used to
generate the same data.
Positrons deposit energy in the detector in much the same way as do electrons. However, when they
come to rest, through annihilation, two 511-keV photons are released in opposite directions. If either photon
undergoes Compton scattering in the device, then the total positron energy plus the added energy left by
the scattered photon appear summed in the pulse height spectrum. Consequently, a high energy tail can
appear with positron spectroscopy (discussed and shown later in Sec. 20.9). Because Si has a low Z number,
the spectrum from a Si(Li) detector suffers less from Compton scattering effects than do detectors composed
of higher Z materials.

16 The maximum energy listed in Table 16.7 is the energy of the particle whose CSDA range is x. So heavy charged particles
with E < Emax , that mostly travel in straight lines as they slow, are completely stopped within a distance x. By contrast,
the tortuous paths traveled by electrons allow some electrons with E > Emax to still deposit all their initial energy within a
thickness x.
Sec. 16.4. Detectors Based on Group IV Materials 747

The electron backscatter coefficient for Si is relatively small, being approximately 0.14 at 100 keV (see
Fig. 7.7). As discussed in Sec. 7.2.2, the backscatter coefficients in Fig. 7.7 are for the special case in
which the particle enters perpendicular to the surface. However, backscattering becomes worse as the
entrance angle decreases from 90◦ ; hence the backscattering coefficients of Fig. 7.7 depict overly optimistic
results. Regardless, Si is one of the best semiconductor materials for electron spectroscopy.17 To improve
the measured electron energy spectrum the source can be collimated so electrons are normally incident on
the detector. In this manner, improved spectral features can be obtained without excessive backscattering
adding to the low energy tail.
There are special precautionary measures that must be taken for charged particle spectroscopy. First,
to eliminate energy loss from the environment, the particle source and detector should be in an evacuated
vessel. Further, Si(Li) detectors can be operated at room temperature, but better energy resolution is
obtained if the detector is cooled to some extent. Commercial spectrometers often come with an integrated
method of cooling the detector. However, when chilling the detector, precaution should be taken to prevent
condensation forming on the detector itself and, thereby attenuating the incident charged particles. The
prevention of condensation is typically achieved by operating the detector in vacuum. Also, some commercial
units may have a thin window protecting the entrance contact, but such windows add to the overall dead
layer thickness. For spectroscopy of low-energy electrons, it is best to enclose both source and detector,
without a window, in the evacuated chamber. In fact, some commercial vendors offer a Si(Li) detector with
a mount that can be directly attached to a user’s vacuum chamber. For special cases requiring transmission
measurements, where the goal is to measure ΔE for a particle passing through the detector, transmission
devices, sometimes called sidelookers, with thin contacts on front and back are available. Aligning several
transmission Si(Li) detectors can be used to measure electron energies that have ranges beyond that of a
single detector.

16.4.2 Detectors Based on Ge


Germanium (Ge) was first reported as a semiconductor detector by McKay in 1949. This initial Ge detector
was manufactured from a point-contact Ge rectifier, and was reported as a particle counter.18 Ge is a
mature and commercially available semiconductor manufactured in many radiation detector configurations.
With a density of 5.33 g cm−3 and atomic number of 32, it has modest gamma-ray absorption efficiency,
but certainly superior to Si detectors. Ge has a narrow band-gap energy of 0.66 eV at room temperature,
increasing to 0.72 eV at 77 K. Although a narrow band gap has the disadvantage of increasing the thermal
leakage current, it has the advantage of decreasing the average ionization to only 2.98 eV/ e-h pair. Ge has a
cubic FCC lattice formed as a diamond structure. Ge also has an indirect band gap, with a band minimum
at L in the [111] direction (see Fig. 16.27), which helps to increase charge carrier lifetimes, often greater
than 10−3 s for highly pure material. The room temperature charge carrier mobilities are μe of 3900 and
μh of 1900 cm2 V−1 s−1 , which are relatively high. However, Ge detectors are usually operated at 77 K, and
the mobilities are much higher at μe of 39000 and μh of 42000 cm2 V−1 s−1 . A Fano factor below 0.13 is
commonly reported.
Germanium (Ge) Radiation Detectors
Presently, the most popular high resolution γ-ray spectrometers are constructed from high purity Ge (HPGe).
The material is purified through zone refinement, resulting in a nearly intrinsic material. Although numerous
detector configurations exist, including special order devices, a standard unit is a coaxial pπn or pνn design

17 Although both SiC and diamond may have lower backscatter coefficients, these detectors presently do not have the required
active region width for high energy electron spectroscopy.
18 Although Si is the most commonly used semiconductor for electronic components, at one time Ge was widely used for diodes

and transistors. Ge transistors are still preferred for some specialized electronics, such as electric guitar pedals.
748 Semiconductor Detectors Chap. 16

Figure 16.27. The theoretical energy bands of Ge at 300 K calculated with


a pseudopotential method. Data are from Chelikowsky and Cohen [1976].

with the rectifying junction on the outer surface (see Fig. 16.36). The coaxial design permits large detectors
to be fabricated while minimizing the detector capacitance. With the rectifying surface on the outer surface,
rather than on the inner surface, the active volume is increased and detection efficiency for low energy γ-rays
is improved.
One difficulty with HPGe detector operation is the need to chill the device during operation. Because
of the small band-gap energy (0.66 eV at 300 K), the intrinsic carrier concentration of electrons and holes
is much too high at room temperature and significant leakage current is produced when operated at high
voltage, which can damage the detector. For this reason, HPGe detectors are typically attached to a dewar
and cooled with LN2, or they are attached to a low noise refrigerator system. To ensure that damage does
not occur from excessive leakage current should the LN2 be exhausted, most modern systems have a safety
shut-off that disconnects the high voltage if the HPGe detector increases to a preset temperature. Portable
survey detectors and laboratory units are available with either LN2 dewars or electrically cooled refrigerators.
Hybrid LN2/electrical cryostats have become available, in which the main cooler is electrical, backed up with
LN2 cooling in case of a power outage.
The usual standard for quality comparisons of HPGe detectors is to quote the energy resolution for 1.33
MeV γ rays from 60 Co. The expected energy resolution can be approximated by Eq. (16.37), in which the
Fano factor is approximately 0.08. Efficiency, for historical reasons, is quoted most often as a comparison to
a 3 in × 3 in (7.62 cm × 7.62 cm) right cylindrical NaI:Tl detector with the source placed 25 cm from the
face of either detector. For instance, a relative 30% HPGe detector has 30% of the efficiency expected from
a 3 in × 3 in NaI:Tl detector at 1.33 MeV. Although useful as an approximation of detector performance,
due to differences in detector geometries and mounting apparatuses, such sweeping generalizations can be
erroneous for accurate measurements. It is best to characterize the detector efficiency and resolution by
using a method described by ANSI/IEEE 325-1996. A calibrated National Institute of Standards 60 Co check
source is placed 25 cm from the front of the detector face. The number of counts appearing in the full energy
peak for the 1.332 MeV γ ray are divided by the number of emissions over that same time interval, which
Sec. 16.4. Detectors Based on Group IV Materials 749

yields the absolute efficiency. The relative efficiency is found by dividing the absolute efficiency by 1.2×10−3,
which is the standard efficiency for a 3 in × 3 in NaI:Tl detector under the same irradiation conditions.
Li Drifted Ge [Ge(Li)] Detectors
Although Ge was first reported as a radiation detector in 1949 [McKay 1949], it was over ten years later that
it became a serious contender as a radiation detector (spectrometer) [Freck and Wakefield 1962]. Impurity
concentrations were still too high in processed Ge, even for zone-refined materials, in which the background
impurities predetermined the depletion width of diodes and consequently also limited the overall detector
volume. Even at low temperature, a significant density of background impurities would produce high leakage
current. Processed Ge ingots were predominantly p-type from the background impurities. In 1960, Pell
introduced the process of Li drifting, a method to electrically drift Li+ ions through a semiconductor. Li
behaves as an n-type dopant in Ge, and counterbalances the p-type contaminants [Tavendale and Ewan
1963; Tavendale 1966]. Further, Li+ is a small ion and has high mobility in Ge crystals, which allows Li+
ions to be driven deep into a Ge semiconductor block. Li may be applied to one end of a detector with a
grease, oil, or with physical vapor deposition [Goulding 1965; IAEA 1966; Brownridge 1972]. A high voltage
of approximately 500 volts is applied to the crystal by metallic clamps such that the positive Li+ ions drift
into the crystal. The Ge sample is heated to approximately 30-60◦C, usually from the ohmic current, which
can be controlled with thermoelectric coolers. The Li+ ions drift through the lattice as interstitial ions,
individually coming to rest as they neutralize the negative electric field formed by the impurity acceptors,
such that ND +
= NA− [Pell 1960a]. Concurrently, unmatched Li+ ions continue to drift through the lattice
while the voltage is applied. The Li+ drifting proceeds provided that the drift velocity of the Li+ ions is
much greater than the diffusion force, or μLi+ END D∇ND [Pell 1960a]. Hence, Li+ drifting produces a
region of intrinsic behaving material. After the drift process is complete, the crystal is etched and mounted
in a cryostat and evacuated down to at least 10 millitorr. The crystal is then cooled to 77 K, and this
temperature must be maintained at all times whether in operation or not. The Li drifting process enabled
sizeable Ge detectors to be realized, and Ge detectors became a standard for high-resolution gamma-ray
spectroscopy. If the Ge(Li)19 detector warms up, the Li diffuses away from the compensation sites and the
crystal is ruined, no longer performing well as a spectrometer. Because of the problem of Ge(Li) becoming
destroyed if allowed to become warm, which unfortunately happened too often, Ge(Li) detectors have been
almost entirely replaced by high-purity Ge (HPGe) detectors.20

High-Purity Ge Production
If a Ge(Li) detector loses cooling, the Li becomes redistributed through diffusion and an expensive detector
is ruined as a result. This Li redistribution was a serious problem. Although such a damaged crystal could be
redrifted once, maybe twice, the redrifted detector inevitably had poorer energy resolution. Hence, around
1970 an active program began to purify Ge to such levels that intrinsic material was achieved solely through
extreme purification. Two research groups sought to accomplish this purification task, one led by Robert
N. Hall [1971] at the General Electric Company and another led by William L. Hansen [1971] at Lawrence
Berkeley Laboratory [Haller 1996].
The process adopted to purify Ge was originally introduced by Pfann [1952; 1966], referred to as zone-
refinement.21 In zone refining, a series of molten zones are passed in one direction through an ingot. De-
pending on the segregation coefficient of the various impurities, they travel with, or opposite, the direction
of the molten passes. The segregation coefficient is defined as the solute concentration in the freezing solid

19 Pronounced “jelly”.
20 The Li-drifted Si(Li) detector, pronounced “silly” detector, is still in production because the Li ion is immobile at room
temperature and, unlike Ge(Li) detectors, is not ruined if it accidently loses cooling.
21 Sometimes referred to as zone melting or zone leveling, Pfann [1966] clearly distinguishes the differences between the methods.
750 Semiconductor Detectors Chap. 16



 !"#$  

*+, % &% &% 
-$   '()
$






  



 



  










 










 
 





./ 



 -$ 
$



       
 
Figure 16.28. A comparison of HPGe detector performance to that of a 3 × 3 NaI:Tl scintillation detector.
The gamma-ray source is a mixture of 152 Eu, 154 Eu, and 155 Eu.

to that of the concentration in the molten liquid. The segregation coefficient is greater than unity if the
impurity raises the melting point of the material, and less than unity if it lowers the melting point. After
numerous passes of the molten zones, the impurities collect at either end of the ingot, leaving a relatively
pure substance in the middle.
The impure end regions are sliced from the ingot, and the remaining purified material is used to grow
a single crystal of Ge (commonly through Czochralski methods). Impurity levels below 2 × 1010 cm−3 are
common for zone-refined Ge. Although the purified material is nearly devoid of impurities, the finished
product is usually slightly p-type (denoted π-type) or slightly n-type (denoted ν-type). The single crystals
of high-purity Ge (HPGe) are then sliced into sections and ground to a desired shape, typically a cylinder.
The grinding and slicing damage to the crystal is subsequently etched away and p and n junctions are applied
to the sample to produce p-π-n or p-ν-n diodes.
The gamma-ray absorption efficiency for Ge (Z = 32) is much less than that for the iodine (Z = 53)
in NaI:Tl. Due to the higher atomic number and generally larger size, NaI:Tl detectors often have higher
detection efficiency for high-energy gamma rays than do HPGe detectors, but much poorer energy resolution,
as shown in Fig. 16.28. When first introduced, Ge detector efficiency was commonly compared to that of
a 3 inch diameter × 3 inch long (3 × 3) right circular cylinder of NaI:Tl for 1332-keV gamma rays from
60
Co. Even today, efficiency of a Ge detector is quoted in terms of a 3 × 3 NaI:Tl detector (Fairstein et
al. 1996). For instance, an HPGe detector denoted as 60% relative efficiency has 60% of the efficiency that
a 3 × 3 NaI:Tl detector would have for 1332-keV gamma rays from 60 Co. HPGe detectors are much more
expensive than NaI:Tl detectors, hence are best used when gamma-ray energy resolution is most important
Sec. 16.4. Detectors Based on Group IV Materials 751

for measurements. If efficiency is of greatest concern, it is often wiser to use a NaI:Tl detector. Comparison
spectra between a 20% HPGe detector and a 3 × 3 NaI:Tl detector are shown in Fig. 16.28. Although very
expensive, modern manufacturers do produce larger HPGe detectors with 200% relative efficiency.
Various Designs
HPGe detectors are manufactured in various shapes, although most conform to either a planar or coaxial
design. Small detectors are commonly manufactured as planar detectors. Relatively large HPGe detectors are
manufactured as coaxial devices mainly to keep detector capacitance low. Small HPGe detectors usually have
better energy resolution than larger devices, and the larger detectors have better γ-ray detection efficiency.
Planar HPGe planar detectors are typically fabricated by applying a doped region upon a highly pure slab
of Ge so that the abrupt junction approximation is valid. The solutions for the electric field and the width
of the depletion region were derived in Sec. 15.3. The electric field was determined to be
|qe |Nb
E(x) = − (W − x), 0 ≤ x ≤ W, (16.53)
κ0
where W is the depletion region width, Nb is the net background doping concentration, κ is the semiconductor
dielectric constant, and 0 is the permittivity of free space. The depletion width, as a function of applied
voltage, is
1/2
2κ0 (Vbi − V )
W  , (16.54)
|qe |Nb
where Vbi is the junction built-in potential. The full depletion voltage is obtained by setting W = WD ,
|qe |Nb WD
2
VD = Vbi − . (16.55)
2κ0
Remember that VD is a reverse (negative) voltage by convention. If the applied reverse voltage is higher
than the required depletion voltage, then the electric field becomes
|qe |Nb |V − VD |
E(x) = − (WD − x) − , V > VD . (16.56)
κ0 WD
Coaxial The electric field in a coaxial detector can be found by solving Poisson’s equation for a cylinder
with space charge
 
1 ∂ ∂V 1 ∂2V ∂2V −qe (NA− + ND+
+ n + p)
∇2 V = r + 2 2
+ 2
= , (16.57)
r ∂r ∂r r ∂φ ∂z κ0
where κ is the semiconductor dielectric constant, 0 is the permittivity of free space. For the following analy-
sis, assume that the detector is a straight coaxial cylinder, thereby eliminating the angular and longitudinal
dependences of φ and z. Under operation, it is assumed that the device is fully depleted of charges, leaving
behind a net space charge, denoted here as ρc . Eq. (16.57) reduces to
 
1 d dV (r) d2 V (r) 1 dV (r) ρc
r = 2
+ =− , (16.58)
r dr dr dr r dr κ0
The rectifying contact is usually fabricated on the outer surface of a coaxial detector, although it could
also be formed on the inner surface. The choice of placing the pn junction on the outer surface allows the
depletion region to increase from the largest geometric volume, easily understood by approximating

Δv  2lπrΔr (16.59)
752 Semiconductor Detectors Chap. 16

where Δv is an incremental change in volume, l is the coaxial length, Δr is a incremental increase in radius,
and r is a radial distance located between r1 and r2 . Here r1 is the coaxial inner radius and r2 is the outer
radius. The volume incrementally increases the most where r is the largest, i.e., at r2 .
HPGe coaxial detectors are usually operated with the high voltage applied to the outer contact, with the
inner contact held at ground potential. For gas-filled coaxial detectors, the high voltage is almost always
applied to the central wire with the outer cylinder wall held at ground potential. However, because the
actual Ge crystal is contained in a vacuum sealed protective housing, the high potential is not accessible to
the user. Hence, the high voltage is applied to the outer contact at r2 , with the electronic readout connected
to the contact at r1 . This bias configuration reduces electronic noise introduced into the input FET (at r1 ).
To solve Eq. (16.58) first use the change of variable r = ey , from which
dV dV dy dV −y
= = e , (16.60)
dr dy dr dy
and  
d2 V d2 V dV
= e−2y − . (16.61)
dr2 dy 2 dy
Substitution of Eq. (16.60) and Eq. (16.61) into Eq. (16.58) then yields the equation
d2 V ρc 2y
2
=− e , (16.62)
dy κ0
whose general solution is
−ρc e−2y
V (y) = + C1 y + C2 . (16.63)
4κ0
Substitution of r = ey back into Eq. (16.63) yields
−ρc r2
V (r) = + C1 ln(r) + C2 , (16.64)
4κ0
where C1 and C2 are arbitrary constants.
The values of C1 and C2 can be found in terms of the boundary voltages V (r1 ) and V (r2 ). In terms of
V0 = V (r2 ) − V (r1 ), C1 is found to be
ρc r22 − r12
V0 −
κ0 4
C1 = , (16.65)
r2
ln
r1
and C2 is
ρc r22 − r12
V0 −
ρc r12 κ0 4
C2 = − ln(r1 ). (16.66)
4κ0 r2
ln
r1
Hence, at full depletion of the HPGe volume, the voltage distribution in the HPGe crystal is
ρc r22 − r12
V0 −
−ρc r2
κ0 4 r
V (r) = + ln (16.67)
4κ0 r2 r1
ln
r1
Sec. 16.4. Detectors Based on Group IV Materials 753

Figure 16.29. Calculated electric field profiles for a HPGe detector


with r1 = 0.4 cm and r2 = 2.5 cm. The background impurity con-
centration is |NA − ND | = 1010 cm−3 . The calculated minimum full
depletion voltage is 1554 volts. Also shown is a comparison to the
calculated electric field within a Ge(Li) detector of the same size.

and the corresponding electric field is

ρc r22 − r12
− V0
dV κ0 4 ρc r
E(r) = − = − . (16.68)
dr r2 2κ0
r ln
r1

If the electric field just barely reaches the contact at g rays g rays
r1 , then the device is said to be fully depleted. Hence,
with the condition E(r1 ) = 0, the voltage required for
diffused Li implanted
full depletion is, n-type contact p-type contact

 2 
ρc r2 − r12 r2 r2
VD = − 1 ln . (16.69)
κ0 4 2 r1

An example of the electric field expected in an HPGe


detector of average dimensions is shown in Fig. 16.29
compared to that expected from a Ge(Li) detector of
the same size and dimensions. Note that the weighting
potential for both the HPGe and Ge(Li) detectors is the
implanted diffused Li
normalized field distribution of the Ge(Li) detector. p-type contact n-type contact
Coaxial detectors are usually fabricated as blind
right cylinders, in which the coaxial center hole is not Figure 16.30. Typical configurations for π-type and ν-
drilled completely through the cylinder. The blind sec- type coaxial HPGe detectors.
tion of the detector is used as the entrance window, a geometry that serves to increase the gamma-ray
absorption efficiency. However, for a right circular cylinder, the electric field strength around the detector
edge perimeter is weak and causes reduced charge carrier velocity, usually observed as longer pulse rise times.
754 Semiconductor Detectors Chap. 16

To remedy the problem, blind coaxial detectors are bulletized (end is rounded) to even out and increase the
electric field strength around the edge (see Fig. 16.30).
The capacitance of a straight coaxial HPGe detector can be determined from the depletion depth. For a
simple coaxial capacitor, the difference in potential from the inner conductor to the outer conductor can be
found from  r2  
V0 r2
V = dr = V0 ln  , (16.70)
r1 r r1
where the undepleted region may be too conductive to behave as a dielectric; hence, r1 is the depletion
region boundary. The total charge at the depletion boundary is
 L  2π
κ0 V0
Q= dz r1 dφ = 2πLκ0 V0 , (16.71)
0 0 r1

where L is the cylinder length. Capacitance is defined as C = Q/V0 , hence, at full depletion, it is obvious
that the capacitance per unit length becomes,
C 2πκ0
= . (16.72)
L ln (r2 /r1 )

Pulse Shape
Determining the pulse shape for planar detectors is relatively straightforward. At 77 K, the hole mobility
is higher than the electron mobility, with μe = 36000 cm2 V−1 s−1 and μh = 42000 cm2 V−1 s−1 , giving a
μe /μh ratio of 0.875. Consequently, it takes 1.143 times longer to collect electrons over the same distance
as holes. It is expected that holes are collected faster than electrons, linearly, with electric field. From
Eq. (8.44) the charge induction, without trapping, for a planar detector is

dQ qe qe E
= [ve + vh ] = [μe + μh ] (16.73)
dt W W
while both types of charge carriers are in motion. Otherwise, as one charge carrier is collected, and the other
is in motion, only one charge carrier type contributes to the induced current. If only electrons are in motion,
dQ qe μe E
= , (16.74)
dt W
and if only holes are in motion,
dQ qe μh E
= . (16.75)
dt W
Normalized to the total current
  te th
W dQ μe  μh 
=  +  , (16.76)
qe E(μe + μh dt μe + μh  μe + μh 
0 0

where te is the electron collection time and th is the collection time for holes. Substitution of the 77 K
mobilities for Ge, the normalized pulse increases as
  te th
 
W dQ  
= 0.4615 + 0.5385 . (16.77)
qe E(μe + μh dt  
0 0
Sec. 16.4. Detectors Based on Group IV Materials 755

cathode
(p+ contact)
5

2 4
Q0
4 3 1 5

pulse height
h
hole
3 transport
e
electron
transport
2

time
1
th te
anode
(n+ contact)

Figure 16.31. The expected position-dependent pulse


shapes from a planar HPGe detector operated at 77 K.

Ballistic deficit from the RC time constant notwithstanding, the position dependent pulse shape is depicted
in Fig. 16.31. If the event occurs at the anode, then the entire pulse is dependent upon hole collection,
extending to the maximum hole collection time of th . Similarly, if the event occurs at the cathode, then the
entire pulse is dependent upon electron collection, extending to the maximum electron collection time of te .
The pulse shape of a coaxial HPGe detector is much more complicated, a consequence of both the non-
uniform electric field and the non-uniform weighting potential. If the electric field through the device is high
enough to reach velocities near saturation, the pulse shapes can be predicted primarily from the weighting
potential, assuming no trapping complications. The normalized induced charge for a coaxial detector is given
by Eq. (8.80), namely
  −1   
Q(t) r2 r
= ln ln 2 . (16.78)
Q0 r1 r1
where r1 and r2 are the free charge carrier locations after moving from the initial starting location at r0 .
By substitution of r − r0 = vt into Eq. (16.78), the pulse shape of a p+ πn+ detector, where electrons are
collected at the outer contact, is described by
  −1    t   t 
Q(t) r2 ve t  e vh t  h
= ln ln 1 + − ln 1 − , (16.79)
Q0 r1 r0 0 r0 0

where te and th are the electron and hole collection times, respectively. An example of the expected pulse
shapes, as calculated from Eq. (16.79), is shown in Fig. 16.32 for a p+ πn+ HPGe detector operated at
saturation velocity (107 cm s−1 ). For a p+ νn+ HPGe detector, the roles of electrons and holes are switched
in Eq. (16.79).
Cryogenics and Cooling
HPGe detectors no longer need to be constantly chilled to low temperature as did the older Ge(Li) detectors.
However, they still must be chilled to cryogenic temperatures during operation to suppress thermal leakage
current. Otherwise, the energy resolution is poor and the detector may suffer severe damage from excessive
thermal leakage current. Modern HPGe detector units have a thermal sensor that turns off the detector
voltage if the detector temperature rises too high, which can happen if the coolant is allowed to expire or
756 Semiconductor Detectors Chap. 16

Figure 16.32. The expected position-dependent pulse shapes


from a coaxial HPGe detector operated at 77 K, determined from
Eq. (16.79). The calculation was performed for a p+ πn+ detector
with r1 = 5.85 mm and r2 = 33.5 mm. The start locations are iden-
tified as r0 = 30 mm, 20 mm, and 10 mm for locations 1, 2, and 3,
respectively.

prematurely boils off from vacuum failure in the dewar/stem assembly. This thermal sensor precaution is
added to prevent severe damage to the preamplifier circuit. Cooling is achieved by two common methods.
The first is the incorporation of a cryogenic dewar filled with liquid nitrogen (LN2). The second is a
mechanical refrigerator unit operating on a modified Stirling cycle.
The HPGe detector crystal is mounted inside a mounting cup with standoffs to hold it in place. Usually
the mounting cup is electrically attached as an outer contact to the crystal and a conductive pin is used as the
inner contact within the hollow penetration. The mounted crystal is placed inside a housing, hermetically
sealed, and evacuated. Older designs had the entire stem and housing evacuated; newer designs use a
modular approach, in which only the detector compartment is evacuated. In the newer designs, an insulator
plug partitions the electronics from the evacuated detector chamber. In either case, the detector crystal is
shielded by the mounting cup and the housing, which unfortunately reduce efficiency for low-energy gamma
rays. It is common to include a package of molecular sieve in the evacuated chamber to absorb residual gas
molecules when the chamber temperature is lowered. The mounted detector is attached to a cold stem that
is inserted into an LN2-filled dewar. The dewar is lined with “superinsulation”, made of multiple thin sheets
of aluminized Mylar R
, to reduce LN2 losses and lengthen the time between periodic refills. The cold finger is
usually made of copper, and is axially located inside a vacuum-tight jacket. This jacket is also partially filled
with molecular sieve, used to getter residual gas molecules at low temperature. The preamplifier electronics
are stationed close to the detector to reduce line capacitance. In many models, the preamplifer is situated
adjacent to the detector house. In modern modular models, the entire preamplifier is situated next to the
detector within the housing (see Figs. 16.33 and 16.34).
The actual detector is much smaller in size than the housing, and often not exactly a perfect cylinder.
From experience, some detectors may have a small section sliced from the crystal (to remove a twin or bad
region). The actual spectroscopic performance is within the vendors specification, as is the quoted efficiency.
However, casual solid angle calculations without taking into account possible geometry differences produces
measurement error. The accepted method of calibrating a HPGe detector is documented in IEEE 325-1996
[Fairstein et al. 1996], which mostly negates problems with detector shape and size.
Sec. 16.4. Detectors Based on Group IV Materials 757

thin aluminized
cap window mylar HPGe
vacuum
detector
high voltage
mounting cup
molecular center contact
sieve electronics (first FET)
vacuum preamplifier
seal electrical
housing feedthroughs
alternate
LN2 fill/vent
preamplifier
tubes
location
neck tube LN2 transfer
collar

vacuum cold dewar


insulator finger

LN2

molecular
sieve

“superinsulation” in vacuum

Figure 16.33. A common configuration for an


HPGe detector is the vertical dipstick.

LN2 loss of about 15 to 45 ml per hour is expected, although the loss rate can change with environment.
Common 30 liter laboratory dewars are refilled at least every two weeks to avoid accidents or other problems.
Measurements should not be conducted during refills to avoid microphonics noise that could ruin the results.
If the dewar becomes damaged, such that the insulation is compromised, unusually fast boil-off may occur.
A cross section diagram of a common HPGe dewar system in the vertical dipstick configuration is shown
in Fig. 16.33. Alternative configurations include the horizontal dipstick (“side looker”), downlooking device
with the detector pointing down positioned under the dewar, the sidelooking detector attached near the
bottom of the dewar, and the “J” type detector with detector attached near the dewar bottom, but the
detector and housing positioned to point upwards. There are smaller dewars for portable units, usually
rated for approximately 24 hours of use. Some modern dewar systems use a combined system between a
refrigerator and conventional LN2 cooling. These units have a refrigerator that recycles the LN2 boil-off
back into the LN2 dewar. In the case of a power outage, the LN2 keeps the system cool for up to a week.
Because of the recycling of the LN2 in the chamber, these detectors can go without refilling for over a year.
In the last decade, major improvement with mechanical coolers have allowed modern HPGe detectors to
operate without LN2, a convenience for locations where LN2 is hard to come by. Originally, these mechanical
coolers were used to bring the HPGe detector down to operating temperature (∼ 77 K), and then switched
off during a measurement, a procedure requirement because vibrations would cause excessive microphonic
noise that would compromise the spectrum. However, vast improvements in refrigerator design now allow
these systems to continue operation during a spectroscopic measurement. Some laboratory systems have a
large compressor with an umbilical cooler attachment that couples to a modular HPGe detector. Portable
758 Semiconductor Detectors Chap. 16

high center electrical


voltage contact feedthroughs preamplifier

HPGe
crystal
cold finger

cap cold finger


mounting attachment
cup vacuum housing
vacuum seal

Figure 16.34. X-ray image of an HPGe detector mounting and electronics


configuration for a side-looking detector.

units have either modified Stirling cycle refrigerators or pulse tube refrigerators. In either case, the modern
units have negligible vibrations and can operate without LN2.

Detection Efficiency, Absorption Losses, and Dead Layers


The response functions for ν-type and π-type HPGe detectors are quite different at low energies. High
purity π-type detectors are fabricated with Li, an n-type dopant, as the rectifying contact diffused at a
depth of approximately 700 μm thick around the outer surface. A much thinner implanted junction of
p-type dopant (typically boron), approximately 300 nm deep, is formed as the ohmic contact on the inner
surface. Consequently, the relatively thick “dead” layer formed by the outer contact significantly reduces
the detector sensitivity to low energy photons (typically below 40 keV). From Eqs. (16.78) and (16.79),
the reverse bias configuration and geometry of pπn HPGe detectors cause the average output pulse to be
dominated by hole motion. These pπn HPGe detectors typically have slightly better energy resolution at
high γ-ray energies than pνn HPGe detectors.
High purity ν-type detectors are fabricated with p-type dopants implanted and activated at a depth of
approximately 300 nm for the outer rectifying contact. A much thicker diffused Li junction up to 700 μm
thick is fabricated as the ohmic contact. As a result, low energy γ rays and x rays encounter less “dead”
layer in the outer contact, thereby increasing the efficiency for these low energy photons. To take further
advantage of the thin surface contact, these ν-type detectors are typically packaged in a can that has a thin
Be window, thereby minimizing γ-ray and x-ray attenuation through the detector container. An additional
advantage with ν-type HPGe detectors is their increased radiation hardness to neutron radiation. Neutron
damage tends to form hole trapping sites, hence the electron dominated pulses from ν-type HPGe detectors
are somewhat less affected.
In order to reduce absorption losses from low-energy gamma rays, the front window of the detector
cap is fabricated from thin low-density material, commonly aluminum approximately 1.5 mm thick. Alu-
minum windows are used for efficient transmission of energies above 30 keV. However, detectors with special
composite carbon windows or beryllium windows can be purchased that allow transmission for low-energy
gamma rays and x rays down to 10 keV and 3 keV, respectively. Depending on the vendor and the design,
the detector mounting cup may have an open end design, or instead may have a thin aluminized Mylar R

window, apparently in place to reduce infrared absorption. The HPGe crystal is kept in vacuum, which
insulates the cryogenically cooled crystal from the external environment. Otherwise, ice crystals can form on
Sec. 16.4. Detectors Based on Group IV Materials 759

Table 16.8. Typical gamma-ray energy resolution of a few represen-


tative commercially available HPGe semiconductor detectors. Many
other sizes are offered by the different vendors.
HPGe relative energy FWHM
comments source∗
detector eff. (%) (keV) (keV)

20 .715–.975 LN2 cooled B,C,O,P


p-type
50 122 .9–1.2 LN2 cooled B,C,P
coaxial
100 1.2–1.4 LN2 cooled B,C,O,P

20 1.8–2.0 LN2 cooled B,C,O,P


p-type
50 1332 1.9–2.1 LN2 cooled B,C,P
coaxial
100 2.0–2.3 LN2 cooled B,C,O,P

20 .69–1.0 LN2 cooled C,P


n-type
50 122 .86–1.2 LN2 cooled C,P
coaxial
70 1.1–1.3 LN2 cooled C,P

20 1.8–2.0 LN2 cooled C,O,P


n-type
50 1332 2.1–2.3 LN2 cooled C,O,P
coaxial
70 2.3–2.5 LN2 cooled C,P
∗B = Baltic Scientific, C = Canberra, O = Ortec,
P = PGT (now defunct).

the cap, and in the worst case, inside the cap on the actual detector. The vacuum is also necessary to reduce
the accumulation of contaminants on the Ge crystal surface. Over time, an accumulation of contaminants
adhering to the Ge surface can increase the detector leakage current, a value that must be maintained below
20 pA during operation. Because the detector windows are thinned at the front entrance, these detectors are
designed for irradiation from the front. Note that gamma rays may enter from the sides with relatively good
efficiency for moderately high energy gamma rays, yet the user should be aware that detection efficiency
changes between front irradiation and alternative orientations.
Detectors to be used primarily for low energy measurements need not have a large block of germanium
to accomplish the task, nor is the coaxial configuration required. Instead, the planar design is used, with
effective diameters available between 6 mm to 70 mm and ranging between 6 mm to 20 mm thick. The planar
detectors are pνn devices, with an outer p-type implanted contact to reduce the dead layer. The edges are
not bulletized, but instead maintain 90◦ edges, which improves the efficiency of gamma-ray measurements
for sources placed close to the detector face. These detectors have better overall absorption efficiency than
a Si(Li) detector because of the higher Z (32 opposed to 14); however, they suffer a noticeable decrease in
absorption efficiency at 11.1 keV from the Ge K-edge, a fact that should be taken into consideration when
deciding on a type of detector for low energy gamma-ray measurements.
As previously stated, the standard reporting procedure for efficiency calibration is outlined in IEEE
Standard 325-1996, and efficiency is reported for 1.33 MeV gamma rays from 60 Co as a comparative ratio to
that of a 3 in × 3 in right circular cylinder NaI:Tl detector [see Fairstein et al. 1996]. HPGe detectors can
be obtained commercially with efficiencies ranging from 10% up to 200% [Sangsingkeow et al. 2003], with
expense significantly increasing with efficiency. Energy resolutions for some commercially available HPGe
detectors are listed in Table 16.8.
Efficiency response examples for a few HPGe variations are shown in Fig. 16.35. Notice in Fig. 16.35 the
dip in efficiency at the Ge K absorption edge (11.1 keV). Also note the efficiency reduction below 100 keV
for the p-type HPGe detector, which becomes only an issue for the n-type devices represented in Fig. 16.35
760 Semiconductor Detectors Chap. 16

at energies below 10 keV. The drop in efficiency is due to a combination of photon absorption in the detector
contact dead region and the container holding the detector. Detectors specifically designed for low energy γ-
ray spectroscopy typically have thin Be windows that do not appreciably attenuate γ rays entering the device.
Overall, the decision regarding which HPGe detector is best for an application requires some knowledge of
the preferred energy resolution, necessary detection efficiency, and the photon energy range of interest.
Radiation Damage
Radiation interactions in Ge can cause displacement damage. Under common use, charged particles typically
cannot penetrate the detector housing, and gamma-ray damage is minimal. It is damage from fast neutrons
that can cause degradation in detector performance by producing Frenkel defects that give rise to charge
carrier trapping. Consequently, HPGe detectors operated in radiation fields with appreciable fast neutron
exposure suffers, over time, from performance degradation, manifested as a trapping tail (Sec. 15.5.1) and
broadening of the energy resolution.
These damage induced defect sites preferentially trap holes over electrons. Consequently, coaxial ν-type
detectors are less susceptible to radiation damage effects than coaxial π-type detectors. This difference can
be understood by inspecting the geometric weighting and the weighting potential of the detectors. Recall
from Eq. (16.59) that the outer detector volume has a higher probability of gamma-ray interactions than
inner portions, obvious from volumetric arguments. A π-type detector has the rectifying barrier on the
outside perimeter, and holes are drifted in the direction of r2 → r1 . With a linear dependence of r, the
geometrical dependence indicates that more hole dominated pulses appear than electron dominated pulses.

Figure 16.35. The absolute detection efficiency for several HPGe detector
configurations with a 2.5 cm source to end cap spacing, showing a (A) 200
mm2 × 10 mm thick low energy ν-type nominally planar HPGe detector, (B)
10 cm2 × 15 mm thick low energy ν-type nominally planar HPGe detector, (C)
coaxial π-type HPGe detector with 10% relative efficiency, (D) coaxial thin
window ν-type 15% relative efficiency HPGe detector, and a (E) broad energy
range π-type 5000 mm2 × 30 mm thick nominally planar HPGe detector. After
Canberra, Incorporated [2016].
Sec. 16.4. Detectors Based on Group IV Materials 761

a b c d
n-type Li diffused
p-type implantation
surface barrier
passivation

e f g h

Figure 16.36. Different commercially available HPGe detector structures


with electric field lines depicted: (a) basic planar detector, (b) grooved planar,
(c) low capacitance planar, (d) surface barrier planar, (e) truncated pνn blind
coaxial, (f) pνn blind coaxial, (g) nπp blind coaxial, (h) pπn well configuration.
After Darken and Cox [1995], Canberra [2016] and Ortec [2016].

From the coaxial design, the induced current is highest as charge carriers drift in the vicinity of r1 (see
Sec. 8.7). Under severe hole trapping, holes originating from the outer regions near r2 may not reach r1 ,
and consequently, the pulse output is compromised and lower than expected, producing low energy tails for
energy peaks in pulse height spectra.
The opposite case is true for ν-type detectors, for which the majority of pulses are electron dominated.
Because the neutron induced defects are primarily hole traps, electron transport from r2 to r1 is less affected
by charge carrier losses. Holes drifting from r1 towards r2 may suffer from trapping, but most of their
induced charge is produced in the region nearest r1 . Hence, holes can still contribute a significant amount
to the induced current before they are lost to traps.
Both devices can be heated and annealed to remove neutron radiation damage. Detectors manufactured
from ν-type Ge can be annealed at approximately 100◦ C for one day to effectively remove defects. However,
π-type HPGe detectors must be annealed at slightly higher temperature (∼ 120◦ C) for up to a week to
effectively remove neutron induced defects. Unfortunately, because Li is used as the n-type dopant on the
outer surface of π-type HPGe detectors, the high diffusivity of Li allows it to drive deeper into the detector
and increase the outer surface dead region. Consequently, the low energy sensitivity of π-type detectors
reduces with the annealing procedure. However, the implanted p-type contact on the outer surface of ν-type
detectors is not affected by diffusion at the relatively low annealing temperatures, and consequently does not
suffer a reduction in low energy efficiency. In short, ν-type HPGe detectors are better suited for operation
in a fast neutron environment than are π-type HPGe detectors.

Detector Structures
There are several types of HPGe detector structures available for specific uses. These structures include
detectors optimized for low energy gamma-ray measurements, specifically designed with thin dead regions
and thin entrance windows. Other detectors are optimized for best energy resolution, increased radiation
hardness, or high detection efficiency. Some of the more popular structures are depicted in Fig. 16.36 and
discussed in the following sections.
Although detection efficiency is mostly determined by the detector volume, the energy resolution is a
function of the statistical fluctuations in the production of electron-hole pairs, charge carrier losses during
762 Semiconductor Detectors Chap. 16

Figure 16.37. Example of energy resolution dependence on gamma-


ray energy, electronic noise, and trapping. The curves for the total
and the trapping FWHMs were found with a linear least squares fit
and the curve for the eh pairs FWHM was modeled with F = 0.06
in Eq. (16.83). Data are from Owens [1985].

transport, and signal fluctuations from electronic noise, so that


 1/2
2 2 2
FWHM = (FWHMnoise ) + (FWHMtrap ) + (FWHMeh ) . (16.80)

The contribution from statistical fluctuations in excited charge carriers is presumed Gaussian in nature, the
variance in number of charge carriers produced is

2 F Eγ
σeh = = F N̄ , (16.81)
w

where Eγ is the gamma-ray energy, w is the average excitation energy, F is the Fano factor correction
constant, and N̄ is the average number of charge carriers produced. The fractional standard deviation is
 <
F Eγ 1 wF
σeh(f ) = = , (16.82)
w N̄ Eγ

and by multiplying this fraction by the original gamma-ray energy, the contribution of the excited charges
to the energy resolution is found as
 
FWHMeh = 2 2 ln(2)σeh(f ) Eγ = 2.355 wF Eγ . (16.83)

Contributions from electronic noise can generally be measured with a pulser added into the circuit under
normal detector operation, usually through a connection port provided on the preamplifier. The value of
FWHMnoise can be measured from the resulting pulse height spectrum of the pulser input. Sources include
the detector and line capacitance, possible ground loops, and impedance mismatch of connectors.
Sec. 16.4. Detectors Based on Group IV Materials 763

As seen in Sec. 15.5.1, the pulse height spectrum is skewed towards a lower energy tail, an effect that
is important for high trapping losses. Hence, the FWHM is not strictly Gaussian in nature.22 Further, the
contribution from charge carrier trapping changes with detector voltage and size. Larger detectors suffer
more trapping, and consequently a higher variance contribution. Increasing the voltage can reduce the effect
of trapping, but with limited results. Ultimately, charge carriers reach a saturation velocity (see Fig. 16.5),
and increasing the voltage actually has an adverse effect if electronic noise increases. Further, at high
enough voltages the diode can reach a voltage breakdown condition. Manufacturers usually have a suggested
optimum voltage that produces the best overall energy resolution.
Overall, the total energy resolution FWHM of HPGe detectors, in units of energy, increases with gamma-
ray energy. This dependence becomes obvious from Eq. (16.83) for the FWHM in electron-hole pairs pro-
duced, but should also be intuitive from the trapping consequences described in Sec. 15.5.1. As the gamma-
ray energy increases, the photon absorption becomes more uniform, which decreases the energy resolution
in the presence of trapping. Note also from Fig. 16.37 that electronic noise has more effect on resolution for
low-energy gamma rays than with high-energy gamma rays.
Planar Detectors The physical attributes of planar semiconductor detectors have been presented in Chap-
ter 15 and in prior sections of this chapter. Of particular note is that planar structures are much easier
to fabricate than coaxial detectors. However, the linear weighting potential of a planar detector is more
susceptible to resolution degradation from charge carrier trapping. Fortunately, HPGe detectors have low
trap densities, long charge carrier lifetimes, and high charge carrier mobilities at low temperature. It is found
that smaller planar HPGe detectors yield better energy resolution, with many quoted as having a resolution
of less than 200 eV FWHM at 10 keV. HPGe detectors designed for low energy gamma-ray spectroscopy do
not need large active volumes, and hence, do not need to be configured in a coaxial structure. Planar HPGe
detectors have special use as low energy gamma-ray spectrometers; however, because of their reduced mass,
they are considerably less efficient than coaxial detectors at high gamma-ray energies. Shown in Fig. 16.36
are three common planar structures, the simple planar, the grooved planar and the low capacitance planar
structures. The grooved structure (Fig. 16.36(b)) suppresses the surface leakage current and thus reduces
electronic noise. The small electrical contact design shown in Fig. 16.36(c) takes advantage of a reduced
detector capacitance, non-linear weighting potential, and high energy-resolution typical of a small detector
to improve performance at low energies. All of the shown planar configurations have a shallow p-type im-
planted region on ν-type material which serves as the rectifying contact and entrance surface. Coupled with
a low Z thin cap window, these detectors can be used for gamma-ray and x-ray energies down to 3 keV.
With low Z polymer window materials [Moxtek 2017] as replacements for beryllium windows, it is possible
to detect photons with energies below 1 keV. A relatively new configuration fabricated from π-type material
has a Schottky barrier front contact, a Li diffused n-type contact around the periphery, and a small p-type
contact at the collection electrode. This detector type can have outstanding efficiency and energy resolution
performance at energies ranging from 3 keV up into the higher energy range generally relegated to coaxial
devices (see Figs. 16.36 and 16.38).
Coaxial Detectors By far the most popular geometry in current use, the coaxial detector design offers out-
standing energy resolution and gamma-ray detection efficiency. Capacitance is reduced from common planar
detectors, as already mentioned. Coaxial detectors are fabricated from either ν-type or π-type materials,
both having advantages. Coaxial pπn detectors generally have better energy resolution performance than
coaxial pνn detectors of similar size, but the thick dead region formed by the Li-diffused junction limits

22 Owens[1985] argues that HPGe coaxial detectors have nearly Gaussian features even in the presence of trapping provided
that the applied electric field is high. This observation is perhaps true, but takes advantage of the coaxial geometry with the
non-linear weighting potential, for which the charge carriers suffering higher trapping are collected on the outer electrode.
764 Semiconductor Detectors Chap. 16

Figure 16.38. Energy resolution at FWHM as a function of gamma-


ray energy for several commercial HPGe detector types identified in
Fig. 16.36. Data are from Canberra [2016].

detection to gamma-rays above 40 keV. Coaxial pνn detectors can be used for lower energy gamma-ray
detection, down to 3 keV, and they are much more radiation hard to neutrons than their nπp counterparts.
The configuration is harder to manufacture than a common planar detector. Straight coaxial detectors have
a hole, usually 8 mm to 10 mm diameter, drilled and etched straight through a right circular cylinder. Blind
coaxial detectors have the hole drilled nearly through, but with approximately 5 mm of mass left at the
detector end. Recall that blind coaxial detectors have the end bulletized to help produce a uniform electric
field in the device. The detectors are designed for front side irradiation, and can be acquired in a number of
different dewar/detector configurations, the most popular are the dipstick and the top side-looker. Shallow
coaxial detectors (Fig. 16.36 (e)) have lower capacitance from the smaller size and are generally thicker than
most planar designs. These shallow coaxial detectors are fabricated as pνn devices, allowing their use for
low-energy gamma-ray spectroscopy with better energy resolution than their larger coaxial counterparts.
Unfortunately, because of their smaller size, truncated coaxial detectors have reduced efficiency at higher
gamma-ray energies.

Well Detectors The well detector, shown in Fig. 16.36 (g), is a device that nominally produces a 4π
counting geometry, in which the radiation source is placed inside the well structure. To achieve highest
performance at low energies, the well hole is doped with p-type implants in a π-type blind coaxial device.
The outer surface is doped with diffused Li to produce a n-type contact. For this configuration, it must be
fully depleted to take advantage of the thin p-type implanted ohmic junction. The construct of the well cap
is thin aluminum, usually thin enough to allow detection down to 10 keV. Because of the geometry, well
detectors suffer compromised energy resolution compared to other geometries, but can still achieve FWHM
near 3 keV for 1332-keV gamma rays. There have been some commercial well hole units in the past that
were true coaxial detectors, with the hole drilled completely through the detector. The configuration of the
blind hole well requires a longer lead to the first amplifier stage which is manifested in microphonic noise
[Gilmore 2008]. The lead on a through-well structure can be shorter, thereby reducing the electronic noise
problem. Although the loss of mass at the bottom of the well may reduce efficiency, this problem can be
mitigated by making the coaxial detector longer.
Sec. 16.4. Detectors Based on Group IV Materials 765

Special HPGe Detectors HPGe detectors can be fashioned into numerous different geometries for
application-specific measurements. For instance, special instruments for high energy physics [Eberth and
Simpson 2008], Compton scatter studies [Choong et al. 2008], gamma-ray tracking [Wieland et al. 2003], and
gamma-ray imaging [Niedermayr et al. 2005] have been built for these various applications. In some cases,
an array of common coaxial HPGe detectors may be adequate, although the geometry of the array may
require innovative electronics arrangements. These arrays improve efficiency and reduce Compton scattered
photon losses while yielding information of the gamma-ray trajectories. Eberth and Simpson [2008] provide
a good review of several detector array projects and results for assemblies of commercial HPGe detectors.
The maturity of germanium crystals enables the production of segmented arrays of detectors that come
in many forms. The most basic are large crystal volumes snuggly fit into a single package and interconnected
to form a single device. For instance, the CLOVER device introduced by Canberra Industries [Canberra
2012] has four detectors that when connected provide over 130% efficiency at 1.33 MeV by using a coinci-
dence counting method to sum the full energies of Compton scattered and pair production events. Other
segmented detectors have been fashioned by defined sections on either planar and coaxial detectors through
photolithography methods [Sandsingkeow et al. 2003], or by directly cutting grooves with a wire saw [King
et al. 2008]. In either case, the end result is an array of rectifying contacts individually isolated on the outer
surface regions. Cylindrical detectors are divided into zones, and individual preamplifiers attached to these
zones are used to sense independent signals originating from these zones. By doing so, Compton scatter
imaging and gamma-ray tracking can be performed. Commercial manufacturers offer segmented detectors
in either planar or coaxial geometries, some with over 30 segments to a single coaxial device. Segmented
detectors can also be arranged in complex arrays to increase the total volume of a detection system.

16.4.3 Diamond Detectors


Another single element group IV semiconductor used occasionally as a radiation detector is carbon in the form
of diamond. Diamond was the first semiconductor investigated, successfully, as a radiation detector [Stetter
1941], although it went largely unnoticed at the time. Diamond forms as an FCC lattice,23 has an indirect
band gap of 5.47 eV, and requires on average 13.25 eV to produce an electron-hole pair. Overall, the high
ionization energy results in fewer charge pairs produced per unit energy than either Si or Ge. Consequently,
there is a reduction in relative pulse height for diamond detectors compared to other semiconductors, yet the
average ionization energy is still approximately two to three times less than most gases used in proportional
counters. With a Z of only 6, it is the lightest of the group IV semiconductors. The dielectric constant of
diamond is relatively low at 5.7 and the index of refraction is 2.424 at a wavelength 546 nm, reducing to
2.418 at 500 nm. The atomic density is 1.763 × 1023 cm−3 and the mass density is 3.52 g cm−3 .
Diamond has a thermal conductivity coefficient of 25 W cm−1 K−1 , which is nearly 17 times greater
than silicon. The room-temperature electron and hole mobilities for natural diamond reach 2800 and 2000
cm2 V−1 s−1 , respectively. Shown in Figure 16.39 are variations of charge carrier mobilities with temperature
and impurity concentration. Near 300 K, these mobilities are only slightly altered with changing temperature.
From the literature, highly doped diamond suffers reduction in mobility at low temperature, not an intuitive
result [Nebel 2003].
The room-temperature charge carrier saturation velocities are higher than most semiconductors, reaching
velocities greater than 1.6 × 107 cm s−1 for electrons and greater than 107 cm s−1 for holes (see Fig. 16.40).
Because of its low Z, it is impractical as a gamma-ray spectrometer; however, it has found use on occasion
as a particle detector, especially for high-temperature applications. Having a Mohs hardness of 10, it is also
more radiation resistant than all other semiconductors. Diamond has a displacement energy ranging between

23 It
is often classified as a diamond lattice, but this is actually incorrect terminology. Instead it is the FCC Bravais lattice with
two atoms arranged at each lattice point.
766 Semiconductor Detectors Chap. 16

 

  1 / N np   T 1
    !"#

   !"
 
  T 1.5


$% 
$% 
  

$% 
 &   # 

#$% 
#$%
#$% 
 
             

       

Figure 16.39. The charge carrier mobility in diamond as a function of (left) impurity concentration and
(right) temperature. Data are from Nebel [2003].

Figure 16.40. The charge carrier velocity in pure natural diamond as a


function of electric field and crystal orientation. Data are from Nava et al.
[1980] and Reggiani et al. [1981].

35 and 48 eV per atom depending on the irradiation direction in the crystal [Bourgoin and Massarani 1976;
Koike et al. 1992], higher than common semiconductors used for radiation detection. The displacement
energies for most semiconductors generally range between 6 to 25 eV per atom [for examples, see Loferski
and Rappaport 1959; Larin 1968; Bryant and Cox 1968]. This radiation resistance should not be interpreted
as being radiation proof, because diamond also accumulates displacement damage from charged-particle and
neutron interactions. Consequently diamond detectors also suffer eventual catastrophic failure in a harsh
Sec. 16.5. Compound Semiconductor Detectors 767

radiation environment. However, the onset of failure from charged particle damage is usually at a much
higher fluence, approximately an order of magnitude greater than observed with either Si or Ge.
Diamond is synthetically produced by chemical vapor deposition (CVD) in a microwave chamber, gen-
erally limited to a thickness of 1 mm or less [Hemley et al. 2005]. The process requires a reaction between
hydrogen and methane gases at low pressure and at a relatively high temperature, typically above 700◦ C
[Schwartz et al. 2004; Wolfer et al. 2009]. The concentration of methane is much lower than the hydrogen,
usually only 1-2% of the total gas mixture [Liang et al. 2009]. The organic gas molecules decompose in the
microwave field and deposit the carbon in layers on a prepared substrate, after which a post-growth anneal
at higher temperatures (> 2000◦C) eliminates graphite structures that may have formed [Liang et al. 2009].
Growth rates increase with temperature, and apparently growth rates also increase with the introduction of
nitrogen [Yan et al. 2002]. Including a small amount of oxygen in the CVD plasma also increases the growth
rate of diamond, improves crystallinity, and suppresses the formation of graphite [Tapper 2000]. CVD-grown
diamond reportedly has higher mobilities than natural diamond, reaching up to 4500 cm2 V−1 s−1 for elec-
trons and 3800 cm2 V−1 s−1 for holes [Wort and Balmer 2008]. Effective doping of diamond is difficult, but
can be performed. The ionization energies of traditional dopants in group IV materials are relatively large.
For instance, the ionization energy of boron (p-type dopant) is 0.37 eV and the ionization energy of arsenic
and phosphorus (n-type dopants) are 0.41 eV and 0.59 eV, respectively. Regardless, pn junction diodes have
been successfully produced with diamond. Except for impure materials, a rectifying junction is probably
unnecessary for diamond detectors because the intrinsic resistivity is greater than 1013 Ω cm.
The construction of diamond detectors is simple, usually consisting of a parallel plate design with metal
contacts on opposing surfaces. Alternative designs have a pair of interdigitated electrodes on a single surface
[Mainwood 2000]. One of the major advantages of diamond is its relatively higher radiation hardness to other
semiconductors. Because the band gap is wide and also indirect, the probability of band-to-band radiative
transitions is low. Instead, performance is strongly dependent on the trap density, and Shockley-Read-Hall
recombination dominates. The radiation hardness of diamond is usually measured by the degradation in
charge collection efficiency, defined by a comparative decrease in the combined charge carrier drift lengths,

λe + λh = (μe τe∗ + μh τh∗ )E = ve τe∗ + vh τh∗ . (16.84)

In other words, as defects are introduced through radiation absorption events, the trap density increases and
the mean free drift time (τ ∗ ) decreases. The overall induced charge loss is also a function of detector thickness.
Hence, it is expected that as the thickness of a diamond detector is increased, the relative radiation hardness
decreases. Damage tends to become severe for charged particle fluences exceeding 1015 cm−2 [Mainwood
2000], an order of magnitude higher than observed for Si [Adam et al. 2000] and bulk GaAs [Gersch 2002].

16.5 Compound Semiconductor Detectors


Compound semiconductors have been under investigation since 1945 when Van Heerden first explored the
use of AgCl as a radiation counter. Unfortunately, compound semiconductors have been substantially less
successful than group IV semiconductors. One main reason for the lower success is because of increased
number of possible defects that can form with compound semiconductors, commonly arising from antisite
defects and non-stoichiometric effects, neither of which is a problem with common group IV semiconductors
such as Si and Ge. Added to the complications with purification, these multiple defects can increase charge
carrier trapping and affect the electric field profile. However, there are a few compound semiconductors that
are useful for special applications, a few of which are described in the following sections.
Compound semiconductor detectors have become more important in recent years, with commercial units
now available. Typically these detectors are somewhat smaller than Si- and Ge-based detectors, mainly due
to material imperfections. Regardless, a few materials, namely CdTe, CdZnTe, and HgI2 , have desirable
768 Semiconductor Detectors Chap. 16

properties for room-temperature operated devices, an advantage not shared by Si(Li) or HPGe detectors.
The reason for this advantageous property is that, at 300 K, their larger band gap energies reduce their
intrinsic carrier concentrations and substantially increase their resistivities. Further, CdTe, CdZnTe, and
HgI2 all have relatively high Z atomic constituents, hence have larger gamma-ray absorption coefficients
over those of Si and Ge. Still, because of their typical smaller size, energy resolution for these compound
semiconductor detectors are usually reported relative to 662-keV gamma rays of 137 Cs instead of 1.33 MeV.
Because of the importance of these properties, lengthy reviews have been periodically published that are
devoted entirely to the status of compound semiconductors as radiation detectors, notably Hofstadter [1949a;
1949b], Chynoweth [1952], Mayer [1966], Sakai [1982], Cuzin [1987], Squillante and Shah [1995], McGregor
and Hermon [1997], and Owens and Peacock [2004]. Further, a few technical books have devoted much
material to discussions on compound semiconductor radiation detectors, such as Bertolini and Coche [1968],
Schlesinger and James [1995], and Owens [2012]. In the present text, the authors attempt to condense
that vast amount of information on compound semiconductor radiation detectors to a manageable level,
incorporating some of the more important developments and findings.
The total charge collected is usually affected by crystalline imperfections that serve as trapping sites, which
are energy states that remove free charge carriers from the conduction and valence bands. Charge is induced
as long as these charge carriers are in motion; hence, their removal diminishes the output voltage. Although
the actual trapping process is complicated, it is typical to describe the relative charge collection efficiency as
a simplified function of trapping. The induced charge for planar detectors is given by Eq. (15.240), which is
written here as    
Q(x) x−W −x
= e 1 − exp + h 1 − exp , (16.85)
Q0 e W h W
where W is the detector active region width, Q0 is the initial excited charge magnitude, x is the event
location in the detector, and    
τe,h ve,h μe,h τe,h V
e,h = = , (16.86)
W W2
where τ is the charge carrier lifetime, v is the charge carrier velocity, and V is the applied operating voltage.
Note, that the relative charge collection is dependent upon the interaction location x, and for low values of
, the energy resolution can be poor. Good energy resolution is achieved if  > 50 for both electrons and
holes, for which Q/Q0 has little deviation over the detector width W . In some cases, even if the value of 
is low for one charge carrier (holes, for instance), energy resolution can often be preserved by irradiating the
cathode side of the detector provided that the gamma-ray energy is relatively low, below the energy at which
the cross sections for Compton scattering and photoelectric effect are equal. The reason for the preserved
energy resolution is because electron-hole pairs are predominantly produced near the cathode, thereby most
of the induced charge is from electron motion.24 For more penetrating gamma rays, the effect diminishes as
electron-hole pairs are produced more uniformly over the detector bulk.
The value of  can be increased by decreasing the detector size (W ), increasing carrier lifetimes (τ ) through
material improvement, or increasing the applied voltage V . Due to practical voltage limitations and the
fundamental difficulty with improving materials, most compound semiconductor detectors are manufactured
with small active widths to improve detector energy resolution, and, hence, the devices are relatively small.
The μτ values for electrons and holes are often quoted measures of quality for compound semiconductors
used as γ-ray spectrometers.
Several other methods have been employed to improve the performance of compound semiconductor
radiation spectrometers. Electronic correction methods aimed at addressing charge loss have been used,

24 If h  e , seldom the case, then one should obviously irradiate the anode instead of the cathode.
Sec. 16.5. Compound Semiconductor Detectors 769

which include pulse-height rejection and pulse-height correction methods. Advanced detector designs that
manipulate the weighting potential to effectively turn the detectors into “single carrier devices” have also
been used to improve energy resolution. In more complex systems, a combination of weighting potential
manipulation combined with pulse height correction have been used to produce excellent results. Examples
of these methods are described in the following sections.

16.5.1 SiC Detectors


SiC is a group IV compound semiconductor that has long been inves-
A tigated as a potential radiation detector. SiC has a density of 3.21 g
B
cm−3 with atomic numbers 14 and 6. SiC can form in over 200 different
polymorphs, and the first identified polytype was a rhombohedral lat-
C tice (15R) [Ott 1925; Thibault 1944a, 1944b]. The three most common
commercial forms of SiC are 4H, 6H, and 3C. The number indicates the
repetitive layering sequence and the letter indicates the Bravais lattice,
H for hexagonal, R for rhombohedral, and C for cubic.25 The structural
unit of SiC is a tetrahedron with four carbon atoms about a Si atom,
although the basis can be considered the Si-C pair. Each of these pairs
is located at a lattice point. A layer of the basis type can be formed in
a two-dimensional hexagonal close pack lattice, such as a rack of billiard
Figure 16.41. In a close pack lat-
tice, layers can stack in positions A, balls (see Fig. 16.41), which can serve for reference as the basal plane
B, or C. The sequence by which atoms labeled A. A second layer can be laid atop the depressions of the first
stack upon these locations determines layer, of which there are two possibilities, labeled B and C. Essentially all
the polymorph.
of the SiC polytypes can be assembled by arranging these three possible
layering structures in a proper sequence.
From Fig. 16.41, a 2H SiC polytype has stacking sequence ABAB where AB is the repetitive sequence.
In similar fashion, the 4H polytype has sequence ABCB, the 6H polytype has sequence ABCACB, and the
3C polytype has sequence ABC (zinc blende) [Iwami 2001]. Although the mass densities are the same for
these polytypes, the band-gap energies are not: the band gap for 3C is 2.36 eV, for 6H is 3.05 eV, and for 4H
is 3.23 eV. SiC is also extremely hard with a Mohs hardness of 9. At 9.66, SiC has a slightly lower dielectric
constant than most semiconductors. The intrinsic resistivity of 4H SiC is greater than 1015 Ω cm. SiC has
a high melting point (decomposition point) of 2830◦C (3100 K), a temperature that precludes traditional
melt growth methods of production. Instead, SiC bulk crystals are grown by vapor phase transport (VPT),
chemical vapor deposition (CVD), or liquid phase epitaxy (LPE) [Dmitriev and Spencer 1998; Sudarshan et
al. 2005]. Vapor epitaxial methods are used to grow high quality SiC layers, usually on a bulk SiC substrate.
With any of these methods, the production costs are relatively high, thereby making SiC wafers expensive
by comparison to most other semiconductors.
Because SiC has such low Z numbers, it is relatively uninteresting as a gamma-ray detector. With the
wider band gap, 4H SiC has an average ionization energy of approximately 7.8 eV per electron-hole pair, much
larger than the average ionization energy of Si at 3.6 eV per electron hole pair. Further, the high temperature
properties and the chemical resistance of SiC make pn junction formation a challenge, requiring much higher
temperatures (greater than 2000◦C) than that needed for common Si diode fabrication [Saxena and Steckl

25 Ramsdell [1947] suggested this classification method rather than the previous arbitrary method of designating SiC types in
sequential order of discovery. Instead, the number represents the number of layers per unit cell and the letter designates the
Bravais lattice; H for hexagonal and R for rhombohedral. Thibault [1944a] named the cubic polytype β-SiC and named all other
polytypes α-SiC with Roman numeral designations. Because there is only one cubic form, Ramsdell kept the identification
β-SiC, yet even this was eventually changed to C for cubic. Hence, Type I became 15R, Type II became 6H, Type III became
4H, Type IV became 3C, etc.
770 Semiconductor Detectors Chap. 16

2500
55 4 +100°C 13.9 SiC pixel detector
Fe 5.9 keV Pulser
10 Pulser
17.8 241

2000 6.3 Am
T = +30 °C
2.0 7.9
5.3 9.6 16.9
11.8
3 +27°C 20.8
10 15.8
1500
Counts

Counts
196 eV FWHM 113 eV FWHM 21.4 26.35
(6.1 el. r.m.s.) 22.1
1000 2
10

500 6.49 keV Pulser line width:


177 eV FWHM (9.6 el. r.m.s) @ +100°C
1
10 120 eV FWHM (6.5 el. r.m.s) @ +27°C
0
4.5 5.0 5.5 6.0 6.5 7.0 7.5 8.0 0 4 8 12 16 20 24 28
Energy (keV) Energy (keV)

Figure 16.42. (left) Spectrum of 55 Fe acquired at 100◦ C with a SiC pixel detector. An 8 μs triangular
pulse shaping was used and the electronic noise was 8.9 electrons r.m.s. (right) Comparison spectra of
241 Am acquired at 27◦ C and 100◦ C with a SiC pixel detector. From Bertuccio et al. [2011]; copyright

Elsevier (2011), reproduced with permission.

1998]. Junction devices can be formed with CVD epitaxial growth of doped layers or with ion implantation
of dopant species. Because pn junction formation introduces fabrication complications, Schottky contacts
are a common method of producing rectifying junctions on SiC substrates. Ohmic contacts generally require
a doped sublayer of material, produced by CVD or implantation, before the ohmic metal is applied. The
hardness of SiC also presents a challenge for chemical and plasma-based etching. Surfaces that terminate
with either C or Si atoms have different chemical properties.26
Regardless, there are several attributes to SiC that are of interest for radiation detection. First, because
of the high melting point and the wide band gap, SiC detectors can be operated at high temperatures (greater
than 700◦C) with negligible leakage current [Babcock et al. 1963]. Second, it is relatively radiation hard by
comparison to most other semiconductors [Babcock 1965; Barry et al. 1991; Kinoshita et al. 2005; Ruddy
et al. 2007; Lefévre et al. 2009]. Hence, a thrust for SiC detector research is for high temperature radiation
environments, such as those found in the vicinity of a nuclear reactor [Dulloo et al. 1999]. Third, SiC has a
high thermal conductivity coefficient 4.9 W cm−1 K−1 at room temperature. Fourth, SiC has a saturation
velocity of 2 × 107 cm s−1 , nearly twice that of Si. Finally, SiC has a high breakdown electric field, 2.2 × 106
V cm−1 for 4H material and 2.5 × 106 V cm−1 for 6H material so that high voltages can be applied to the
detectors. Of the commercially popular SiC polytypes, 4H has emerged as the favored material for radiation
detectors mainly because it has higher charge carrier mobilities than 6H and much higher resistivity than
3C. SiC wafers up to 150 mm diameter can be acquired commercially.27 Because epitaxial SiC is generally
of higher quality than bulk SiC, it is common that a high-quality epitaxial layer, grown upon a bulk grown
SiC substrate, serves as the detection volume.
SiC has been studied as a neutron detector since the early 1960s [Brussels 1960; Weisman 1960, 1962;
Belgium 1962; Babcock et al. 1963]. The primary reason for interest in SiC is because it has unique properties
that permit their operation at high temperatures in a harsh radiation environment [Canepa et al. 1964;
Seshadri et al. 1999; Nava et al. 2008; Ha 2009]. Detectors for slow neutron detection are usually fashioned
as pn or Schottky junction diodes coated with a converter material [Dulloo et al. 2003; Manfredotti et
al. 2005; Ha et al. 2009]. A type of SiC fast neutron detector relies on fast 12 C(n,n )12 C and 28 Si(n,n )28 Si
elastic and inelastic collisions, along with numerous possible threshold reactions, as the detection mechanisms
[Ruddy et al. 2006a; Ha et al. 2011]. Ruddy et al. [2006a] show spectral features for several fast reactions in
a 4H SiC pin structure, and also demonstrate different pulse height spectra from three different fast neutron

26 This trait is common to compound semiconductors.


27 Cree, Inc.
Sec. 16.5. Compound Semiconductor Detectors 771

sources, 252 Cf, AmBe, and a D-T generator. An alternative fast neutron detection method is to cover the
SiC diode with a hydrogenous material such as HDPE and use the (n,p) recoil reactions as the detection
method [Flammang et al. 2007]. A more detailed discussion about these neutron detectors is reserved for
Chapters 17 and 18. Ruddy et al. [2006b] report on the performance of 4H SiC material as an alpha particle
detector. These detectors were fabricated from a 100 micron thick high purity SiC epitaxial layer grown upon
a 300 micron thick n-type SiC substrate. Ruddy et al. [2006b] report room temperature energy resolution
of 41.5 keV FWHM at 3.18 MeV and 55.4 keV at 8.38 MeV. SiC has also been studied for low-energy x-ray
detectors [Bertuccio et al. 2004a, 2004b, 2011; Moscatelli 2007; Nava et al. 2008]. Although these detectors
are not suitable for high energy gamma-ray detectors, they performed well for photon energies below 60
keV. Bertuccio et al. [2004a, 2004b, 2011] report on photon detectors fabricated from SiC epitaxial layers,
nominally 70 microns thick, grown upon SiC substrates. Operated at 373 K, energy resolution of 233 eV
FWHM has been reported for 5.9-keV gamma rays for a pixel detector with a 200 micron diameter Schottky
junction (Fig. 16.42) [Bertuccio et al. 2011].

16.5.2 Detectors Based on Group III-V Materials


Group III-V semiconductors are produced from elements in group III and group V of the periodic table. These
materials include binary compounds such as GaAs, GaP, InP, and AlSb, ternary compounds such as InGaAs
and InGaP, and quaternary compounds such as InGaAsP. For ionizing radiation detector applications, the
binary compounds have been investigated the most, although some ternary and quaternary materials have
been explored, primarily as contact materials. Both GaAs and InP are relatively mature semiconductors
that are in common use within the VLSI industry. Both of these important semiconductors have direct band
gaps and show negative differential resistance at high electric fields. Because of their direct band gaps, these
two semiconductors have been used most commonly for photonic emission devices such as LEDs and laser
diodes. The relatively wide band-gap energies of many III-V semiconductors have motivated researchers to
investigate their potential use as room temperature semiconductor radiation detectors.

GaAs
Gallium arsenide (GaAs) was first reported as a semiconductor detector by Harding et al. in 1960. It is a
relatively mature and commercially available semiconductor with some properties that make it attractive as
a radiation detector [McGregor and Kammeraad 1995]. With a density of 5.32 g cm−3 and atomic numbers
31 and 33, it has similar gamma-ray absorption properties as Ge. It has a band gap of 1.42 eV and, thus,
allows room temperature operation for moderate size detectors. GaAs has a direct band gap, which is
beneficial for photonic emission devices, but also decreases the charge carrier lifetime. Electrons confined
in the direct Γ valley have a high mobility, theoretically up to 8500 cm2 V−1 s−1 and, thus, generate high
electron velocities. The indirect L valley of GaAs is 1.71 eV, as shown in Fig. 16.43, which produces negative
differential resistance as electrons transfer from the Γ valley to the L valley for electric fields exceeding 3×103
V cm−1 (see Fig. 16.6).
The intrinsic resistivity of GaAs is approximately 108 Ω cm, but GaAs detectors still must have blocking
contacts to reduce leakage current to manageable levels. Detectors are most often produced with Schottky
blocking contacts, generally composed of varied thicknesses and combinations of Au, Ti, and Pt [Williams
1990]. Almost all radiation detectors reported were fabricated with 100 GaAs substrates. Consequently,
the 100 surface states typically “pin” the Fermi energy level near mid-gap, thereby largely decoupling the
work function of the metal from the resulting Schottky barrier height. Regardless, there is some experimental
evidence that modest alterations in the energy barrier can be achieved with appropriate surface treatments
and choice of metal contact [Williams 1990]. The alternative to Schottky barrier blocking contacts is the
application of p and n junctions. However, these junctions are not easily achieved with GaAs.
772 Semiconductor Detectors Chap. 16

Figure 16.43. The theoretical energy bands of GaAs at 300 K calculated


with a pseudopotential method. After Blakemore [1982].

Purification through traditional methods, such as zone refinement or zone leveling, are rendered difficult
because arsenic outstreams from GaAs when heated above 400◦C for prolonged periods of time, increasing
in rate with temperature, thereby ruining the material.28 Consequently, impurity purification is performed
on starting materials (Ga and As) before crystal growth, with purity levels exceeding 7N being commercially
available.29 However, high resistivity is usually achieved by deep level compensation rather than intrinsic
properties through purity. Deep level compensation is commonly achieved in bulk GaAs with the antisite
AsGa with As located on a Ga lattice location. This antisite defect produces a double deep donor with
energies, measured at 0.75 eV and 1.0 eV below the conduction band edge, label EL2 [Martin et al. 1980;
Thomas et al. 1984; Bourgoin et al. 1988; Martin and Makram-Ebeid 1992; Baraff 1992].
Historically, GaAs was the first compound semiconductor to demonstrate high energy resolution at room
temperature (295 K) for gamma rays [Eberhardt et al. 1970, 1971]. Those detectors were fabricated with
GaAs crystals grown by liquid phase epitaxy (LPE), a crystal growth method that intrinsically purifies mate-
rials through thermal migration of impurities. Unfortunately, the detectors were also limited to thicknesses
of approximately 130 microns and, thus, severely limiting the gamma-ray detection efficiency. A typical
pulse height spectrum from such a detector at room temperature is shown in Fig. 16.44. The LPE method
of crystal growth is relatively expensive and impractical as a production method for large volume detectors.
Epitaxially grown GaAs detectors have demonstrated excellent energy resolution [Owens et al. 1999], some
with thicknesses up to 200 microns [Alexiev and Butcher 1992]. Attempts to manufacture thicker epitaxial
GaAs have been explored (up to 600 microns), but the authors state that quality was compromised as the
thickness increased [Hesse et al. 1972]. Unfortunately, thin devices combined with the relatively low atomic
numbers of GaAs offer little advantage over alternative higher Z compound semiconductors, such as CdZnTe
and HgI2 .

28 Ifperformed within a sealed ampoule backfilled with As gas, GaAs can be annealed at elevated temperatures. The cooling
method can greatly alter the electrical resistivity of the material [Lagowski et al. 1986].
29 In the usual jargon for purity, an ‘N’ represents a ‘9’ in purity. Hence, 5N (or five nines) pure is 99.999% pure.
Sec. 16.5. Compound Semiconductor Detectors 773

10

Counts per Channel x 10-2


57
Co Source
W-Ka GaAs #11
8
Temp = 295 K Pulser
_..
Bias = 100 V g-122 10
IL = 1 nA
6

4 W-Ka W-Kb
X-Escapes 2.90
2.95
2 g-122, X-Escapes
g-136

0
0 100 200 300 400 500

Figure 16.44. Room temperature differential pulse height spectrum from a


GaAs Schottky diode fabricated from a 75 micron LPE layer. Reproduced
from Eberhardt et al., Appl. Phys. Lett., 17, 427, (1970), with the permission
of AIP Publishing.

GaAs produced by bulk crystal growth methods was also studied during the 1980s and 1990s, also with
limited success [McGregor and Kammeraad 1995]. Motivation for studying GaAs as a radiation detector in-
cluded application as room-temperature operated gamma-ray spectrometers and as a radiation-hard particle
detectors for high-energy colliders [Beaumont et al. 1992, 1993, 1994]. High resistivity GaAs is generally
compensated with either Cr [Cronin and Haisty 1964; Lin and Bube 1976] or with the native EL2 defect
[Martin et al. 1980; Kaminska 1987; Bourgoin et al. 1988]. In either case, the charge carrier lifetimes are
relatively short, on the order of nanoseconds, thereby drastically reducing the useful size of these detectors.
For a bulk GaAs device 130 microns thick, an acceptable energy resolution of 8.83 keV FWHM was achieved
for 122 keV gamma rays [McGregor and Hermon 1997]. Energy spectra from a bulk GaAs spectrometer is
shown in Fig. 16.45. A modest amount of cooling below room temperature produces a dramatic improvement
in performance, as demonstrated by Bertuccio et al. [1997], namely an energy resolution for 60-keV gamma
rays measured with 100-micron-thick bulk-grown GaAs detectors reduced from 15.5 keV FWHM at 295 K to
2.4 keV FWHM at 243 K. Yet, the small size also rendered these devices useful only for low energy gamma
rays. The problem with compensated bulk GaAs is that the field dependent capture cross section of EL2
[Panousis et al. 1969; Prints and Bobylev 1981; Prinz and Rechkunov 1983] alters the electric field within
the detectors and causes the electric field to increase with a non-traditional voltage dependence [McGregor
et al. 1994a].
The deep level EL2 is an intrinsic antisite defect AsGa that naturally produces a double deep donor
with energy levels approximately 0.75 eV and 1.0 eV below the conduction band edge EC . EL2 levels are
neutral when filled with an electron and positively charged when empty. This antisite defect is purposely
produced in concentrations of about 1016 cm−3 by introducing additional As into the GaAs melt source
[Holmes et al. 1982]. A careful balance of the EL2 concentration with that of the residual carbon acceptor
concentration (usually near 1015 cm−3 ), and possibly other acceptor impurities, produces semi-insulating
(SI) material with resistivities of about 108 Ω cm. This relatively high resistivity is still inadequate to
produce resistive devices, and instead SI GaAs detectors are fabricated as rectifying diodes operated under
reverse bias. Under equilibrium conditions, only a fraction of the EL2 deep donors are ionized and the Fermi
level is pinned near midgap, as explained by the three-level model of Sec. 12.5.4. However, as the detector
is reverse biased, the EL2 deep donor becomes fully ionized, and produces excess positive space charge near
the reverse biased junction as shown in Fig. 16.46. Consequently, the non-uniform ionization distribution
promotes the appearance of a two-zone electric field distribution [McGregor and Kammeraad 1995].
774 Semiconductor Detectors Chap. 16

4500 600
241 57
(a)
(a) 59.5 keV Am Source Co Source (b)
4000
GaAs detector Pulser
g-rays 500 GaAs detector 122 keV
3500 T = 21oC T = 21oC g-rays
Counts per Channel

Counts per Channel


Bias = -400 V Bias = -400 V Pulser
3000 Thickness = 130 mm 400 Thickness = 130 mm
2500 8.05 keV 5.9 keV 4.9 keV
FWHM 300
2000
FWHM 8.83 keV FWHM
X-ray FWHM
1500 escapes 200

1000
136 keV
g-rays
100
500

0 0
50 100 150 200 250 50 100 150 200 250 300 350 400 450 500
Channel Number Channel Number

Figure 16.45. Room temperature differential pulse height spectra from a 130 μm thick, 0.5 mm2
bulk SI GaAs detector. From McGregor and Hermon [1997]; copyright Elsevier (1997), reproduced
with permission.

As the bias is increased further, the capture cross section of the EL2 increases [Panousis et al. 1969; Prints
and Bobylev 1981; Prinz and Rechkunov 1983], and increases the likelihood that electrons are recaptured,
thereby effectively neutralizing a fraction of the deep donors [McGregor et al. 1992, 1994a, 1994b]. McGregor
et al. [1994b] propose that the unexpected voltage dependence is a consequence of dynamic trap neutralization
of deep centers from electric field enhanced electron capture. Consequently, a quasi-stable constant electric
field appears which rapidly decreases to low values at the end of the active region. This balance between
trapping and emission at these EL2 sites is a probable reason for low frequency oscillations observed in GaAs
biased at high voltages [Holanyak and Bevacqua 1963; Barraud 1963; Sacks and Milnes 1970; Kaminska et
al. 1982]. This hypothesis is based on an arbitrary “filling function” applied in the model [McGregor 1994a,
1994b], yet measurements by Berwick et al. [1993] seem to confirm the hypothesis. McGregor et al. [1992,
1994a] and Berwick et al. [1993] found that the electric field active region increased nearly linear with applied
voltage, at approximately 1 micron per volt, leaving a considerably wide low-field substrate region with poor
charge collection. Unfortunately, with such a peculiar voltage dependence, it takes 1000 volts to produce a
1-mm-thick active region, a voltage that is impractical for most gamma-ray detector applications. Kubicki
et al. [1994] attempt to explain the unexpected electric field and depletion characteristic by incorporating
leakage currents in their model instead of including the field enhanced capture of electrons. Although the
model has merit in explaining the low-field characteristic, it fails to reproduce the dependencies measured
by McGregor et al. [1992, 1994b] and Berwick et al. [1993]. Similar results to that of McGregor et al.
[1994b] were produced by Cola et al. [1994, 1997], who incorporated the model of McGregor et al. [1994b]
and portions of the model of Kubicki et al. [1994]. Overall, Cola et al. [1997] appear to provide additional
evidence to field enhanced electron capture by EL2 as the cause of the unusual electric field and depletion
characteristic of undoped SI GaAs.
Despite these problems, undoped SI GaAs was found to be useful as a high-speed radiation detector
because of the short charge carrier lifetimes [Wagner et al. 1986; Wang et al. 1986, 1989; Friant et al. 1989].
Detectors of this type were used to measure the radiation wave from nuclear weapons tests. Although these
detectors were capable of following high-speed radiation pulses, response times were still tens of nanoseconds
in duration. The high-speed response was improved by irradiating GaAs materials in a nuclear reactor,
which produced a high density of electron and hole traps than appear in bulk-grown GaAs from the damage,
thereby reducing the response times to 30 picoseconds [McGregor and Kammeraad 1995].
GaAs pixelated detectors have found use for radiation imaging of low-energy gamma rays and x rays
[Manolopoulos et al. 1998; Owens et al. 2001]. The advantages of using GaAs for x-ray imaging over Si
Sec. 16.5. Compound Semiconductor Detectors 775

depleted depleted
compensated compensated
electrons
EC
electrons
EC
++ ++
+++++ EF ++ EFm
+ + + + + +++
+++ ++ E
- - +++++ + + + Fs
- - -
- - - - - - - - - - - - - - - -
Schottky EV Schottky
- - -
Contact holes Contact - - - - - - - - - - - -
EV
filled deep state (neutral) holes
+ empty deep state (ionized)
- filled acceptor state (ionized)

Figure 16.46. Band diagrams of a Schottky contact diode with shallow acceptors and compen-
sating deep donors. (left) With no applied bias, a space charge region appears adjacent to the
Schottky contact. (right) With reverse bias applied, the space charge region extends further into
the semiconductor as more deep donors become completely ionized. After McGregor et al. [1994a].

include the higher density and Z of GaAs, the higher intrinsic resistivity and lower leakage current, the
high Γ valley electron mobility (greater than 8000 cm2 V−1 s−1 ), and pixel isolation is achieved with the
semi-insulating substrate rather than a field oxide. There are other semiconductors with higher Z than
GaAs, such as CdTe, CdZnTe, and HgI2 , yet the maturity of GaAs and the resultant high quality crystal
structure enables common VLSI processing of the pixelated structures.

InP
Indium phosphide (InP) is a compound III-V semiconductor that has received modest attention, sporadically,
as a radiation detector. Perhaps one of the more attractive attributes of InP is its relatively high electron
charge carrier mobility of 4500 cm2 V−1 s−1 , with holes having a mobility of 150 cm2 V−1 s−1 . The saturation
velocity is higher than that of GaAs, reaching over 2.5 × 107 cm s−1 at an electric field of 1.2 × 104 V cm−1 .
The average ionization energy is approximately 4.2 eV per e-h pair. The gamma-ray absorption is dominated
by the higher Z indium component with atomic number 49 (where phosphorus is only 15), and the density
of InP is 4.79 g cm−3 . With a direct band gap of approximately 1.35 eV (Fig. 16.47), the intrinsic resistivity
is approximately 107 Ω cm, just high enough to operate small devices at room temperature. However, this
high resistivity is usually achieved by compensation doping with Fe impurities. Notice from Fig. 16.6 that
InP also possesses negative differential resistance for electrons at electric fields above 1.2 × 104 V cm−1 and,
thus, makes InP attractive for Gunn effect devices.
InP is usually grown by either the liquid encapsulated Czochralski (LEC) method or the vertical gradient
freeze (VGF) method. Undoped material is usually n-type, although resistivity control can be attained by
purposely doping with the n-type dopants S or Sn. InP can be acquired as p-type material if doped with
Zn. High resistivity material is produced by adding a deep accepter compensating dopant to the melt. For
detector purposes, Fe-doped semi-insulating (SI) InP has been investigated the most.
SI InP doped with Fe was explored as a high speed radiation photoconductor to measure short bursts of
radiation. Fe acts as a deep acceptor site and compensates residual shallow donor impurities to produce a
semi-insulating material as described in Sec. 12.5.4. These detectors routinely had response times between
100 ps to 200 ps, determined to be largely dependent upon the bulk recombination of electrons and holes
[Hammond et al. 1981, 1983, 1984]. The response times were shown to be dependent upon the Fe concen-
tration and had an obvious reduction in response time as the deep acceptor Fe concentration was increased
[Wagner et al. 1986]. Wagner et al. [1986] also found that neutron irradiation damage further improved
the high speed response of InP:Fe photoconductors. There is a limit to the neutron damage that can be
776 Semiconductor Detectors Chap. 16

Figure 16.47. The theoretical energy bands of InP at 300 K calculated with
a projector-augmented-wave (PAW) method. Data are from Y-S. Kim et al.
[2009] and Ioffe [2016].

sustained, mainly because the reaction 115 In(n,γ)116 In transmutes into 116 Sn (14.1 s half-life) through β-
particle emission, an n-type dopant for InP and, thus, ultimately reduces the material resistivity over time.
Although the transient response of the detectors was shown to closely follow a short radiation impulse, they
failed to follow the input power of longer duration pulse trains, in particular, square-pulse inputs from a
laser, and instead showed a superlinear response function with elongated tails [Kania et al. 1986; Wagner
et al. 1986]. Neutron irradiation damage failed to show improvement for this particular issue. Wagner et
al. [1986] surmise that the superlinear behavior and observed failure to follow long pulse excitations was
due to an imbalance of electron and hole trapping. Electrons are trapped more efficiently, leading to the
slower moving holes carrying the majority of current. Consequently, steady state output is reached only
when the electron and hole recombination and generation rates become balanced. This same effect dimin-
ishes as the radiation intensity increases. Although these InP:Fe detectors had excellent performance for
transient responses, neutron damaged semi-insulating (SI) GaAs demonstrated faster response times without
the superlinear problem for longer pulses. Consequently, investigation of high-speed InP radiation detectors
diminished in favor of SI GaAs detectors.
InP was also investigated as a possible room temperature semiconductor detector for ionizing radiation
and neutrinos [Lund et al. 1988; Olschner et al. 1989; Suzuki et al. 1989]. These initial investigations
demonstrated that InP:Fe was sensitive to ionizing radiation, although the spectral performance was poor.
The neutrino detection application is generally impractical because of the miniscule solar neutrino cross
section [Raghaven 1976] and would require a rather sizeable InP detector as pointed out elsewhere [McGregor
and Hermon 1997].30 Regardless, this concept continues to be of interest [Fukuda et al. 2010]. As for
detection of ionizing radiation, trapping and the non-optimal resistivity of SI InP leads to poor performance
at room temperature. The charge carrier losses from trapping and the noise from excessive leakage current
[El-Abassi et al. 2001] diminish the signal and cause resolution degradation. Owens et al. [2002a, 2002b]

30 Raghaven[2001] states that a detector with a “modest 4 ton mass of In” would be required, amounting to approximately 1
cubic meter of InP.
Sec. 16.5. Compound Semiconductor Detectors 777

reported improved results for small InP:Fe detectors (3 mm × 3 mm × 0.18 mm thick) used as x-ray detectors.
By cooling the detectors to 213 K to reduce thermal leakage current, Owens et al. [2002a] achieved 2.5 keV
FWHM for 5.9 keV-gamma rays (55 Fe) and 9.2 keV FWHM for 59.5-keV gamma rays (241 Am). By reducing
the detector temperatures even lower to 103 K, Owens et al. [2003b] observed 911 eV FWHM for 5.9-keV
gamma rays and 2.5 keV FWHM for 59.5-keV gamma rays.
From the work of Wagner et al. [1986], it was already observed that Fe compensation reduces the electron
mean free drift times. From Section 12.5.4, it was shown that the concentration of deep acceptors must be
greater than the concentration of shallow donors to produce semi-insulating material. Consequently, there
is a lower concentration limit of Fe that must be introduced to maintain high resistivity and reasonably
low leakage current. Gorodynskyy et al. [2005] and Yatskiv et al. [2009] proposed that Fe doping could be
replaced with alternative co-dopants, such as Ti and Mn or Ti and Zn, and still maintain higher mobilities
and improved charge carrier collection. This hypothesis seems to have merit, in that material produced
by Gorodynskyy et al. [2005] was measured to have over 90% charge collection efficiency (CCE) for 200-
micron-thick devices operated at 250 K with corresponding energy resolution of 3.4% FWHM for 5.48 MeV
alpha particles. However, both CCE and energy resolution were compromised at room temperature (300
K), yielding a CCE of 52% and FWHM of 17% for 5.48 MeV alpha particles. Zdansky et al. [2006] report
on results for small detectors fabricated from Ta-doped InP irradiated with α-particles, which produced
energy resolution of about 6% FWHM at 5.48 MeV. Yatskiv et al. [2009] experimented with InP co-doped
with Ti and Zn instead of Fe to achieve high resistivity material with superior CCE. By designing detectors
with guard rings and cooling the detectors to 230 K to reduce leakage current noise, CCE up to 99.9%
were achieved with a best energy resolution of 0.9% FWHM for 5.48 MeV α particles for 250-micron-thick
detectors. The improved α-particle spectral results indicate material improvement, but remain an impractical
application for InP, mainly because alpha particle backscattering is significantly less for Si detectors than
InP detectors. Because of the relatively poor room temperature performance by comparison to alternative
compound semiconductors, InP radiation detectors continue to be mainly experimental.

16.5.3 Detectors Based on Group II-VI Materials


Group II-VI semiconductors are produced from elements in group II and group VI of the periodic table.
These materials include binary compounds such as CdTe and CdZnTe, perhaps the two most studied II-VI
compounds for radiation detection. The relatively wide band-gap energies of CdTe and CdZnTe allow room
temperature operation of these radiation detectors.

CdTe
Cadmium Telluride (CdTe) is a wide band-gap semiconductor of interest as a room-temperature operated
gamma-ray spectrometer. CdTe has a cubic zincblende crystal structure. CdTe has a direct band-gap
energy of about 1.52 eV, with an indirect L valley of 2.73 eV as shown in Fig. 16.48. A saturation velocity
of approximately 1.5 × 107 cm s−1 is reached at an electric field of 1.5 × 104 V cm−1 , above which CdTe can
also exhibit negative differential resistance much like GaAs and InP (see Fig. 16.6). The average ionization
energy is 4.43 eV per e-h pair with a 0.11 Fano factor. The dielectric constant for CdTe is 10.36 [Strauss
1977]. The wide band gap produces an intrinsic resistivity of 109 Ω cm; however, because of the presence of
contaminant impurities, high resistivities greater than 109 Ω cm are usually achieved through impurity and
defect compensation. CdTe is relatively soft, rating 54 on the Knoop hardness scale (approximately 2.2 on
Mohs scale). The elemental constituents have atomic numbers 48 and 52 and the density of CdTe is 5.86 g
cm−3 . Because of the relatively high Z numbers, photoelectric absorption dominates up to approximately 260
keV. Charge carrier mobilities are 1050 cm2 V−1 s−1 for electrons and 100 cm2 V−1 s−1 for holes. Electron
and hole mean free drift times are material dependent, but often quoted near 3 ×10−6 s and 2×10−6 s,
respectively.
778 Semiconductor Detectors Chap. 16

Figure 16.48. The theoretical energy bands of CdTe at 300 K calculated with
a pseudopotential method. Data are from Chelikowsky and Cohen [1976].

CdTe has been investigated as a room-temperature gamma-ray detector since the mid-1960s [Autagawa
et al. 1967; Mayer 1967; Vavilov et al. 1970; Zanio et al. 1970], and various detailed review articles and books
cover CdTe material and detector performance [Whited and Schieber 1979; Kröger and de Nobel 1955; de
Nobel 1959; Hage-Ali et al. 1995a, 1995b, 1995c; McGregor and Hermon 1997; Owens and Peacock 2004;
Owens 2012]. Because of material imperfections, which include a combination of impurities and native de-
fects, these devices continue to be manufactured as small detectors. Although the band gap is high enough for
room temperature operation, background impurity contamination causes the leakage currents to be too high.
Dopant compensation, typically with Cl, is used to create high resistivity material. Still the detectors must
be manufactured as pn junction or Schottky junction diodes to reduce leakage current to manageable levels.
As a result, the detector volumes are usually no more
than a few millimeters thick. Commercial units are avail-
able as small gamma-ray spectrometers. Typically, the
best energy resolution is achieved with the assistance of
small electronic Peltier coolers.
The melting point of CdTe is 1092◦C and the crys-
tal can be grown through melt-growth processes such as
Bridgman and Stockbarger [Zanio 1978; Hage-Ali and
Siffert 1995a; Lindstrom et al. 2016]. However, Te pre-
cipitates are a chemical consequence of CdTe growth, re-
sultant from the retrograde solubility of tellurium [Zanio
1978]. The CdTe phase diagram shows that the melt
temperature decreases dramatically off stochiometry, es-
pecially salient for Te-rich solutions (Fig. 16.49). Essen-
tially, a higher concentration of Te can be suspended in
Figure 16.49. Temperature versus composition (T -x) di-
agram for the Cd-Te system. After Zanio [1978] and refer-
a mixture of CdTe liquid and solid, which as the mate-
ences thereof. rial solidifies into a CdTe crystal, the excess Te forms
Sec. 16.5. Compound Semiconductor Detectors 779

precipitates in the solid. To reduce the effects of traditional high-temperature melt growth, the traveling
heater method (THM) is commonly used for radiation detector materials. This method has slowly moving
heating coils that travel upwards along a vertical sealed ampoule of Te-rich CdTe stock materials. The Te
melts at a lower temperature (450◦ C) and acts as a solvent for the CdTe stock material. Consequently, the
CdTe stock dissolves at the hotter leading edge of the melt solution and crystallizes at the cooler trailing
edge, much like liquid phase epitaxy. The advantages include a lower process temperature (typically below
900◦ C), lower Te precipitate concentrations, and lower defect and impurity concentrations. However, THM
is a much slower crystal growth method than alternatives, such as high-pressure Bridgman or Stockbarger
growth. CdTe grown by THM is usually doped with Cl, by adding CdCl2 to the stock material, which
compensates native defects and impurities to produce material with high resistivities of about 109 Ω cm.
Ohmic contacts are usually formed with an electroless process, in which noble metal salt solutions of
AuCl3 , AgNO3 or PrCl4 are applied to a polished and etched surface.31 The noble metal salt solution
etches the CdTe surface and displaces Cd from the surface region while redepositing layers of both the
noble metal and Cl [Hage-Ali and Siffert 1995b]. The Cl incorporation can extend beyond 0.5 microns
into the surface [McGregor and Hermon 1997]. Calculations show that ohmic contacts are inadequate to
reduce leakage currents below the induction current produced by radiation events except for small detectors.
Unfortunately, although the resistivity is relatively high, it is still too low to operate CdTe as resistive
devices, and instead must either be fabricated with rectifying blocking contacts or small enough such that
leakage current is minimal. To reduce leakage current while allowing high operating voltages, detectors have
been produced as Schottky junction devices and ion implanted pn and pin devices [Cornet et al. 1970, 1972],
indium diffusion (on p-type material) [Squillante et al. 1989], and LPE growth [Shin et al. 1985].
Although the incorporation of a blocking contact permits higher bias voltages and generally reduced
leakage current, the performance of these spectrometers varied. The rectifying junction causes an imbalance
in the compensation such that deep level ionization produces space charge that ultimately limits the depletion
region depth [Khusainov 1992]. Depletion studies on SI CdTe indicate the presence of non-uniform electric
fields within reverse biased diodes [Malm at al. 1974; Siffert et al. 1978a, 1978b; Hage-Ali et al. 1993]. In some
cases, the electric field did not extend completely across the device until appreciable voltage was applied,
indicating the build-up of a space charge region much like the situation depicted in Fig. 16.46. Polarization
is often observed with Cl compensated CdTe, manifested as a gradual change in gamma-ray sensitivity and
relative pulse height [Siffert 1978a]. Low resistivity CdTe detectors usually suffer less polarization than high-
resistivity detectors, and the problem of polarization can be reduced by using In-doped or low resistivity CdTe
[Whited and Schieber 1979]. Illumination with IR light [Bell et al. 1974] and alternative conductive contacts
have apparently also helped reduce polarization [Bell and Wald 1972; Puschert et al. 1976]. Takahashi et al.
[2002] report on a 2 mm × 2 mm × 1 mm thick CdTe Schottky diode with Pt contacts. In that study, the
CdTe detector had minimal polarization and yielded RT energy resolution of approximately 2.3 keV FWHM
for 59.5-keV gamma rays, decreasing to 810 eV FWHM at 248 K.
CdTe detectors generally suffer from poor hole collection. Consequently, CdTe detectors are usually small
in size, yet the small size also serves to reduce generation current. Regardless, the literature is replete with
examples of excellent room-temperature gamma-ray energy resolution for small devices, usually about 1 to 2
mm thick (see references in [McGregor and Hermon 1997]). Methods to compensate the poor hole collection
problem include single-carrier geometries and electronic correction methods. Hemispherical detector designs
(see Sec. 12.5.2) were explored as room-temperature detectors with good results [Zanio 1977; Siffert 1994; Alt
et al. 1994; Hage-Ali et al. 1995c], resulting in energy resolution of 26 keV FWHM for 662-keV gamma rays

31 Electroless
plating is an auto-catalytic chemical reaction process applied to a surface and does not require the application of
a voltage. The chemical reaction displaces surface ions and causes the deposition of the metal component onto the surface.
De Nobel [1959] provides a description of metal plating processes used on CdTe.
780 Semiconductor Detectors Chap. 16

Table 16.9. Typical gamma-ray energy resolutions of a few rep-


resentative commercial CdTe and CdZnTe semiconductor detectors.
Many other sizes are offered by the different vendors.
area energy FWHM
detector comments source*
(mm2 ) (keV) (keV)

CdTe 9 122 ≤1.2 Peltier cooled


A
Schottky 25 122 ≤1.5 Peltier cooled

CdZnTe ≈ 100 122 ≤6.1 room temp K


hemisphere ≈ 100 662 ≤20 room temp B,K

CdZnTe 100 662 13.2–26.4 room temp


K
coplanar 225 662 16.5–26.4 room temp
∗A = AmpTek, B = Baltic Scientific, K = Kromek.

with a 65 mm3 active volume. Pulse height discrimination (PHD) methods [Jones and Woollam 1975], in
which short pulse heights are eliminated from spectra, help to reduce spectral distortion from hole trapping.
These electronic methods have yielded 7.5 keV FWHM at RT for 662-keV gamma rays for a 5 mm × 5 mm
× 2 mm thick CdTe detector [Richter and Siffert 1992; Richter et al. 1993]. Unfortunately, PHD is a method
that electronically eliminates a sizeable volume of the detector, ultimately reducing the detection efficiency.
The method of pulse height correction (PHC) (charge loss compensation) improves energy resolution while
preserving detection efficiency (see Sec. 15.5.2), where the slope of the pulse rise with respect to time is
used to project the expected true pulse height [Richter and Siffert 1993; Richter et al. 1993, 1993; Eisen and
Horovitz 1994]. Energy resolution of 6.1 keV FWHM and 6.4 keV FWHM for 122-keV and 356-keV gamma
rays, respectively, were achieved by Eisen and Horowitz [1994] with this method. The energy resolution of
commercially available detectors are presented in Table 16.9.
With the relatively good energy resolution of CdTe detectors, they have been demonstrated as detectors
for slow neutrons [Vradii et al. 1977]. The strong neutron absorption cross section of Cd below 0.5 eV (σth
of 113 Cd = 20, 000 b) produces prompt gamma-ray emissions, which can be subsequently detected by the
CdTe detector. Unfortunately, the gamma-ray capture efficiency is low, and the actual neutron detection
efficiency is relatively poor. This type of neutron detector is presented with more detail in Chapter 17.
CdTe detectors are commercially available and have been used for various unique applications for which
small room-temperature gamma-ray spectrometers are best applied. These applications include medical
instruments, heat shield ablation sensors, nuclear power station activity monitors, nuclear fuel probes, cap-
illary electrophoresis detectors, narcotics and explosive scanners, portable dosimeters, ammunition cartridge
control monitors, and various x-ray and gamma-ray imaging devices [see references in McGregor and Hermon
1997]. Small CdTe detectors (5 mm × 5 mm × 1 mm thick), coupled to Peltier coolers having excellent
energy resolution, of about 850 eV at 122 keV, are commercially available [Amptek 2017]. The operating
voltage is nominally 500 volts for these thin devices, thereby requiring cooling below 263 K to reduce the
leakage current to manageable levels.
Cd1−x Znx Te
The introduction of Zn in the growth process of CdTe, nominally between 2% to 15%, has led to the
production of CdZnTe detectors.32 Overall, CdZnTe detectors have the same advantages as CdTe detectors
with several added benefits. By adding a small amount of ZnTe to the melt, many important semiconductor

32 This particular semiconductor is denoted CZT (common), (Cd,Zn)Te (less common), Cd1−x Znx Te, or CdZnTe. By adhering
to traditional elemental symbols, and because of the many different elemental combinations in use for substrates and detectors,
the authors choose to use CdZnTe.
Sec. 16.5. Compound Semiconductor Detectors 781

properties are drastically improved. The band gap of CdZnTe increases with Zn concentration, with band-gap
energy of Cd1−x Znx Te at 300 K is well approximated by [Olego et al. 1985]
Eg (x) eV = (1.51 ± 0.005) + (0.606 ± 0.01)x + (0.139 ± 0.01)x2 eV. (16.87)
The band gap ranges from 1.52 to 1.64 eV for Zn contents ranging from x = 0.02 to x = 0.2; hence the
detectors can operate at room temperature without serious leakage current concerns. With an increased
band-gap energy, the intrinsic free carrier concentration diminishes, thereby increasing the resistivity while
reducing detector leakage current. Butler et al. [1992] report that adding x = 0.2 amount of Zn changes
the resistivity of CdTe from 3 × 109 Ω cm to 2.5 × 1011 Ω cm for Cd0.8 Zn0.2 Te. The dielectric constant
is approximately 10.6 for CdZnTe, although this property is also a function of the Zn concentration. The
addition of Zn increases the hardness of CdZnTe over CdTe and decreases the dislocation density [Anand
2013]. The etch pit density (EPD) is a measure of the dislocation defect density. Butler et al. [1993] show
a marked reduction in the EPD as the Zn content was increased, with the densities of 1.5 × 105 cm−2 ,
104 cm−2 , and 5 × 103 cm−2 for Zn contents of 0, 0.04, and 0.2, respectively. Further, CdZnTe detectors
do not exhibit the polarization phenomenon at low irradiation levels, which are often observed with CdTe
detectors. However, Wang et al. [2013] report the observation of polarization from CdZnTe detectors under
high irradiation conditions. An additional benefit of incorporating Zn is that CdZnTe devices, because of
the increased band gap and resistivity, can be operated at higher temperatures than CdTe devices, and they
can also resolve lower energy photon energies (x rays and gamma rays) traditionally difficult to observe with
CdTe detectors. CdZnTe detectors are presently used in handheld gamma-ray spectrometers and for smaller
medical imaging apparatuses.
The gamma-ray absorption efficiency of CdZnTe is similar to that of CdTe, with a slight decrease in
absorption efficiency with increased concentrations of Zn (Z = 30). The ionization energy is approximately
5 eV per e-h pair, although this number changes as a function of band-gap energy. The Fano factor of
CdZnTe has been measured to be approximately 0.11 [Bale et al. 1999] at 233 K, with at least one research
group [Redus et al. 1997] reporting a lower Fano factor of 0.089 also at 233 K.
Many of the same growth problems with CdTe are also experienced with CdZnTe, including the retrograde
Te solubility. Further, the Zn component has a segregation coefficient larger than unity (about 1.3 at 1100◦C)
and can behave as a migrating impurity during growth, much like a zone-refinement pass [James et al. 1995].
In fact, CdZnTe behaves more like an alloy of CdTe and ZnTe [Owens 2012]. Consequently, there is a Zn
concentration gradient through the crystal ingot that causes a change in the band gap over the length of the
crystal ingot. This gradient appears to be more salient for relatively short ingots over that of long ingots.
Usually, about 2 to 3 cm of material at both ends of the ingot are removed and discarded, and the remainder
is used for detector fabrication. The Zn concentration gradient adversely affects the ionization energy by
increasing the variance in the number of charge carriers excited per unit energy. Consequently, detectors with
a relatively large variance in Zn concentration experience a broadening in spectroscopic energy resolution.
Further, detector shot noise increases with the variance in leakage current, also a consequence of non-uniform
Zn concentration.
CdZnTe substrates were originally developed as low defect substrates with less lattice mismatch for
epitaxial growth of HgCdTe [Bell and Sen 1985; Sen and Stannard 1993], a shallow band-gap semiconductor
used for IR detectors. Variations of Bridgman growth were initially used to grow bulk CdZnTe crystals, as
outlined in James et al. [1995]. However, it was the high pressure method introduced by Raiskin and Butler
[1988] that yielded the material used for the first reported CdZnTe radiation detectors [Butler et al. 1992;
Doty et al. 1992a, 1992b]. For many years, high-pressure (HP) Bridgman growth, pressured with Ar to about
100 atm, was used to produce high-resistivity CdZnTe radiation detectors. CdZnTe material was grown on
the Te rich side of the phase diagram, and as the crystal cooled and solidified in the growth process, Te
precipitates would decorate the grain boundaries in the ingot. Single crystal pieces with low precipitate and
782 Semiconductor Detectors Chap. 16

Figure 16.50. Typical spectrum of 59.54-keV gamma rays from 241 Am taken
with a planar CdZnTe detector. The detector dimensions were 5 mm × 5 mm
× 1.2 mm with a bias of 300 volts. Data from Butler et al. [1993].

defect concentrations were “mined” from the CdZnTe ingots, and these pieces were fabricated into detectors.
Unfortunately, large defect-free pieces were rare, thereby limiting the useful detector sizes. Due to problems
with twinning and the formation of Te precipitates, the useful detector yield with HP Bridgman growth
was poor. Much like CdTe, the traveling heater method is now the preferred growth method for CdZnTe.
CdZnTe can be grown with the THM at lower temperatures (less than 800◦ C). This low temperature growth
reduces the defect concentration, reduces the precipitate concentration, and also reduces Zn segregation.
Although the growth rate is intrinsically limited by the THM method [Peterson et al. 2016], the resultant
product is generally of higher quality than that of HB Bridgman grown material [Roy 2013]. Post-growth
annealing helps to reduce further the size and concentration of Te precipitates.
Large high-resistivity single crystal CdZnTe ingots are now produced commercially for radiation detectors
[Chen et al. 2007, 2008]. Because of the high resistivity, usually greater than 1010 Ω cm, CdZnTe detectors
are manufactured with ohmic contacts instead of blocking contacts and operated as resistive detectors.
Electrical contacts are usually fabricated with electroless AuCl3 , although sputtered Pt contacts have shown
good results.
Planar detectors fabricated from CdZnTe typically have long pulse height spectrum tails (Fig. 16.50), a
consequence of severe hole trapping as described in Section 15.5.1. The severity of the effect increases with
the detector width and gamma-ray energy. Because electron transport is superior to hole transport, CdZnTe
detectors are invariably designed for cathode irradiation, thereby taking some advantage of the increased
gamma-ray absorption nearest the cathode, although the effect diminishes with increasing gamma-ray energy,
as shown in Fig. 16.51.
Most planar CdZnTe detectors are less than 3 mm thick so as to increase the values of e and h . Yet
the poor hole transport properties still produce relatively poor energy resolution for penetrating high-energy
gamma rays. Owens et al. [2002c] show that energy resolution for low-energy gamma rays can be improved by
reducing the detector operating temperature, optimized near 253 K for 59.5 keV gamma rays (see Fig. 16.52).
Sec. 16.5. Compound Semiconductor Detectors 783

Figure 16.51. Comparison spectra taken with a 1 cm × 1 cm area × 2


mm thick CdZnTe detector irradiated on the cathode side with several mo-
noenergetic gamma-ray sources. Charge carrier trapping effects increase with
gamma-ray energy, causing the tailing effect to become more important.

Figure 16.52. The energy resolution temperature dependence of a CdZnTe


detector for 5.9-keV and 59.54-keV gamma rays. The detector was 2.5 mm
thick by 3.2 mm2 area. Data are from Owens et al. [2002c].
784 Semiconductor Detectors Chap. 16

Figure 16.53. Energy resolution of a 1.5 cm × 1.5 cm × 1 cm thick CdZnTe coplanar


grid detector, showing the results with and without electronic depth correction. From
He and Sturm [2005]; copyright Elsevier (2005), reproduced with permission.

Several methods have been introduced to improve energy resolution and efficiency [see review by Zhang et
al. 2013], a few of which are described here. CdZnTe detectors have adequate electron transport properties,
but poor hole transport properties due to the combined effects of short hole mean free drift times and low hole
mobility. As a result, conventional planar detectors seldom produce useful energy resolution for moderate
to high energy gamma rays (greater than 300 keV). Instead, clever geometric detector shapes and electrode
contact shapes are used to modify the weighting potential and electronic signal so that electrons dominate
signal formation rather than holes. Energy resolution below 7 keV FWHM for 662-keV gamma rays can
be achieved at room temperature for these single carrier detector designs. Further, electronic correction
methods are often applied to improve the spectral performance of CdZnTe.
Luke [1994, 1995] introduced the co-planar grid (CPG) CdZnTe detector, described in Sec. 15.5.2, as a
method to remedy poor hole transport. These initial detectors demonstrated superior energy resolution at
662 keV of 24.5 keV FWHM.33 He et al. [1997] used position sensing to improve the energy resolution with
charge compensation methods. He et al. [1998] also demonstrated that an optimized and balanced grid,
including a boundary electrode, on a CPG device yielded superior results, and the use of a balanced grid is
now routine for CPG CdZnTe detectors. He and Sturm [2005] combined the balanced coplanar design with
rise time compensation to achieve room temperature energy resolution of 14.4 keV FWHM at 662 keV for
a 15 mm × 15 mm × 10 mm thick device as shown in Fig. 16.53. Owens et al. [2006] also reported similar
results, but without electronic correction methods, reporting room temperature energy resolution of about
12 keV FWHM at 662 keV.

33 Because CdZnTe detector volumes are relatively small by comparison to most HPGe detectors, the 662 keV gamma-ray
emission from 137 Cs is generally used to report energy resolution rather than the traditional 1332-keV gamma-ray emission
from 60 Co.
Sec. 16.5. Compound Semiconductor Detectors 785

Figure 16.54. Spectroscopic results from 137 Cs for several Frisch collar CdZnTe
detectors, each having a 2:1 aspect ration. The sizes and FWHM resolutions are (a)
0.9% for a 4.7 mm × 4.7 mm × 9.5 mm device, (b) 1.1% for a 6.5 mm × 6.5 mm ×
13 mm device, (c) 1.2% for a 7.8 mm × 7.8 mm × 15.6 mm device, and (d) 2.4% for
a 11 mm × 11 mm × 22 mm device. From Dunn and McGregor [2012].

Quasi-hemispherical CdZnTe detectors were introduced by Butler [Apotovsky et al. 1997; Butler 1997],
and were commercially available for a short time. These detectors were three terminal devices formed on a
parallelepiped CdZnTe block. The detector had a small anode on one surface, and planar cathode on the
opposing surface, and a “control” electrode surrounding the anode [Lingren et al. 1998]. These detectors
performed well, but were usually small. Energy resolution of 3.68 keV FWHM at 511 keV was reported
for a 3 mm × 3 mm × 3 mm device [Butler 1997].34 Parnham et al. [2000] report the development of a
quasi-hemispherical CdZnTe fabricated on a parallelepiped block, on which a top surface has an electrical
contact and the bottom half (approximately) of the remaining five sides of the devices were coated with an
electrical contact. The design worked to improve the energy resolution above that expected from a planar
device, and yielded room temperature (23◦ C) energy resolution of 10.4 keV at 662 keV for a 10 mm × 10 mm
× 5 mm thick device [Bale and Szeles 2006; Szeles et al. 2006].35 Related to the quasi-hemispherical CdZnTe
detector is the ring-drift design [Owens et al. 2007; Alruhalli et al. 2015]. These devices have additional
concentric rings around a central anode instead of the single control electrode described by Butler [1997].
These additional electrode rings enable improved steering of electrons to the anode and help to reduce low
electric field regions present in the Butler [1997] design. Owens et al. [2007] report 4.85 keV FWHM at 662
keV for a 5 mm × 5 mm × 1 mm thick ring-drift CdZnTe detector.
Various quasi-Frisch grid designs were reported by McGregor, including the parallel strip design [McGre-
gor et al. 1998a; McGregor and Rojeski 1998b], the geometrically weighted design [McGregor et al. 1999a;
McGregor et al. 1999b], the Frisch ring design [McGregor and Rojeski 2001; McGregor 2004], and the Frisch
collar design [McGregor and Rojeski 2001; Montemont et al. 2001; McGregor 2004; McNeil et al. 2004]. All
of these detector designs use an external electrode to alter the weighting potential to enhance the contribu-

34 These devices were commercially available for a short while from Digirad.
35 Named CAPtureTM Plus detectors, these devices were commercially available for a short time from eV Products.
786 Semiconductor Detectors Chap. 16

Figure 16.55. Room temperature spectrum of 137 Cs acquired with a CdZnTe pixelated detector (left) without depth
correction and (right) with depth correction. All pixels are summed for both spectra. Bias conditions were -2200 volts on
the cathode and -65 volts on the grid isolating the pixels. c [2005] IEEE. Reprinted, with permission, from Zhang et al.,
IEEE Trans. Nucl. Sci., 52, 2009–2016, [2005].

tion of electron transport to the spectral output. The geometrically weighted Frisch Grid detector combines
orientation, geometrical shape (either a trapezoid or pyramid frustum), the small pixel effect, and the charge
induction isolation of the Frisch grid to produce enhanced energy resolution. These detectors were capable
of delivering room temperature energy resolution of 17.2 keV FWHM at 662 keV for a 1 cm3 device without
electronic corrections [McGregor et al. 1999b]. However, these designs proved difficult to fabricate and led
to simpler permutations, denoted either as Frisch ring or Frisch collar detectors [Kargar et al. 2011a, 2011b;
Harrison 2009] and the basic distinction between the two is described in Sec. 15.5.2. Without electronic
corrections, the Frisch collar design has delivered room temperature energy resolution of 5.9 keV FWHM at
662 keV for a 4.7 mm × 4.7 mm × 9.5 mm device, with comparable energy resolution for larger geometries
(see Fig. 16.54).
CdZnTe has been investigated for medical imaging instrumentation, for which a block of CdZnTe is
patterned with an array of small electrical contacts called pixels. Doty et al. [1994] report on the first
monolithic CdZnTe pixelated device designed for medical imaging purposes. These CdZnTe pixel arrays
were fabricated by traditional VLSI methods. This work led to the discovery of the “small pixel effect”
[Barrett et al. 1995], described in Sec. 15.5.2, and is commonly used to enhance the energy resolution for
gamma-ray spectrometers. CdZnTe pixel devices were successfully used for gamma-ray imaging (examples
include Polichar et al. [1994, 1996], and Barber et al. [1997]). This technology has also proved important
for gamma-ray spectroscopy [He et al. 1999, 2000; Zhang et al 2005]. He et al. [2000] combined CdZnTe
pixel detectors with electronic energy-resolution correction methods to enhance the performance of pixelated
detector arrays (see example in Fig. 16.55). Room temperature energy resolution of 6.16 keV FWHM at
662 keV was achieved with large (1.5 cm × 1.5 cm × 1 cm thick) CdZnTe pixelated detectors [Zhang et al.
2005]. With Compton scatter backprojection methods, these devices can be used to determine the gamma-
ray energy and the general source direction by producing a near 360◦ image of radiation source locations and
include the perceived intensity [Boucher et al. 2012; Wahl et al. 2015]. After many years of development,
these devices are now commercially available.36

36 H3D, Inc.
Sec. 16.5. Compound Semiconductor Detectors 787

16.5.4 Detectors Based on Halide Compounds


The halogen semiconductors are produced from materials with at least one constituent atom from group VII
of the periodic table. These materials include compounds such as HgI2 , PbI2 , and TlBr. Select materials
have wide band-gap energies and can be operated at room and elevated temperatures.

Mercuric Iodide (HgI2 )


Attractive for its large Z components, mercuric iodide (HgI2 ) has long been studied as a gamma-ray spec-
trometer with varying degrees of success [Willig 1971, 1972; Malm 1972; Swierkowsky et al. 1973; Llacer et
al. 1974; Ponpon et al. 1975]. HgI2 has atomic numbers of 80 and 53 with a volume density of 6.4 g cm−3 .
The α-phase (red) of HgI2 has measured charge carrier mobilities of 100 cm2 V−1 s−1 for electrons and 4
cm2 V−1 s−1 for holes [Ponpon et al. 1975]. Thus a substantial voltage is required to ensure acceptably high
charge carrier collection. HgI2 has a measured average ionization energy of 4.42 eV per e-h pair with a Fano
factor of 0.19 [Ricker et al. 1982]. Because of the large atomic number of mercury (80), the photoelectric
effect is predominant for gamma-ray energies below 400 keV (see Fig. 16.1). As a result, HgI2 detectors can
be relatively thinner than other common semiconductors and still have comparable efficiencies. For example,
the absorption efficiency for 140-keV gamma rays in a 2-mm-thick HgI2 detector is similar to 4.2-mm-thick
CdTe or CdZnTe detectors and 1.9-cm-thick Ge or GaAs detectors [McGregor and Hermon 1997]. The
α-phase of HgI2 has a band-gap energy of 2.13 eV and has a resistivity of about 1013 Ω cm.
The melting point of HgI2 is 259◦C, but it also has a relatively low vapor pressure and can be sublimed at
lower temperatures if processed in a vacuum. HgI2 has numerous polymorphs that can form during crystal
growth, most of which are metastable tetragonal structures [Hostettler et al. 2001, 2003, 2005]. The two most
important polymorphs are the preferred α-phase tetragonal crystals (red) formed and stable at temperatures
below 130◦C and the β-phase monoclinic crystals (yellow) that form above 130◦ C. Growing β-phase HgI2
crystals and subsequently cooling them below 130◦C causes a destructive change in the crystals because they
can form any number of metastable crystals or polycrystalline α-phase crystals [Newkirk 1956; Hostettler et
al. 2003]. Moreover, with a melting point of 259◦ C, which is higher than the phase change temperature, a
suitable method to grow detector-quality HgI2 that maintains a growth region below 130◦C is required.
Solution growth methods were first used to grow large HgI2 crystals for radiation detectors [Willig 1971],
and optically clear crystals have been produced with saturated solutions ranging in temperature between
25◦ C and 40◦ C [Mellet and Friant 1989; Nicolau and Joly 1980; Friant et al. 1980]. Unfortunately, detector
performance of these solution grown crystals is compromised by impurity contamination introduced from the
solvent suspension. Because of the improved crystalline quality and the reduction in impurity contamination,
HgI2 vapor growth methods are preferred [McGregor and Hermon 1997]. There are two main methods of
vapor growth, referred to here as the vertical method, initially introduced by Scholz [1974], and the horizontal
method, initially introduced by Schieber et al. [1976].
The vertical method has a relatively large ampoule, typically ranging in diameter between 10 cm to 15
cm and 15 cm high. The bottom of the ampoule has a raised pedestal approximately 3 cm in diameter that
sits atop a temperature controlled cooler region, usually a cold finger or an air jet. The ampoule is either
rotated within a heating coil [Scholz 1974; Schieber et al. 1976] or has a heating framework surrounding
a stationary ampoule [Hermon et al. 1992]. There are three main elements to control the thermal profile
consisting of a controlled cool region under the pedestal, a base heating element around the pedestal, and
an axial heating element. The temperature around and under the ampoule is controlled such that a thermal
gradient nucleates a seed crystal on the pedestal. The process takes several weeks to produce a single crystal
between 250 g to 1000 g.
Schieber et al. [1976] describe an alternate method to growth HgI2 in an evacuated horizontal ampoule
of 5 to 10 cm diameter and 40 cm long. After loading with purified HgI2 materials, ampoules are inserted
into a two-zone furnace with a crystal formation zone held near 103◦ C and other source zone varied between
788 Semiconductor Detectors Chap. 16

1000
241
900
Am 59.5 keV
HgI2 detector g-rays
800 T = 21oC
Counts per Channel

Thickness = 700 mm
700
600 Np X-rays
500
1.9 keV
400 FWHM
300
200

100
0
0 200 400 600 800 1000
Channel Number
Figure 16.56. Room temperature differential pulse height spectrum from a
700-micron-thick HgI2 detector. From McGregor and Hermon [1997]; copyright
Elsevier (1997), reproduced with permission.

8000
Planar (t = 24 hours) Pulsers
Frisch collar (t = 24 hours)
7000 t = Detector bias time at FWHMPlanar = 0.3%
the beginning of counting FWHMFrisch collar = 0.2%
6000
Counts per Channel

2.1 x 2.1 mm2 x L = 4.1 mm


5000 662 keV Counting time (Real): 10 h
Preamplifier: eV550
4000 Amplifier gain: 69X
Shaping time: 1μs
Hg X-ray HV = 1500V
3000 escapes
FWHM = 1.8% ± 0.1%
2000

1000
Source: 137Cs No electronic corrections
0
0 500 1000 1500 2000
Channel Number

Figure 16.57. Pulse height spectra taken with a 2.1 × 2.1 × 4.1 mm3 HgI2 device
with and without a Frisch collar. A 1.8% FWHM energy resolution was measured
with 662-keV gamma rays from 137 Cs when using the Frisch collar. From Ariesanti
et al. [2010]; copyright Elsevier (2010), reproduced with permission.
Sec. 16.5. Compound Semiconductor Detectors 789

97◦ C to 110◦C. The source zone temperature is raised to nucleate a crystal, or is lowered to etch away poorly
formed samples. When one or more good crystals are nucleated, temperature in the source zone is no longer
varied and is held at a temperature above 103◦C to continue the growth of the HgI2 singles crystals. The
process dynamics prevent the growth of crystals larger than approximately 30 g without twinning. Faile et
al. [1980] (also Faile [1981]) simplified the horizontal method by introducing purified HgI2 into an evacuated
growth ampoule approximately 2 to 4 cm diameter and 40 cm long along with low density polyethylene.
This ampoule was inserted into a two-zone furnace with the temperature held at 120◦ C in the source zone
and 100◦ C in the nucleation zone. Several “chance” crystals nucleated and grew near the middle of the
ampoule. The size of these crystals ranged from about a few mm3 to a cm3 in volume and many appeared
as single crystals with better physical and electronic performance than those produced without the addition
of polyethylene.
Faile proposed several hypotheses about how polyethylene aided the growth of HgI2 crystals that included
impurity capturing, ampoule surface priming, free radicals or hydrogen reacting with crystal defects, and
polymers alloying with HgI2 , to name a few [Faile et al. 1980]. However, none of these hypotheses could
explain the observed results. McGregor and Ariesanti [2013] found that the function of low molecular weight
polyethylene is to be a source of polar organic ketone molecules, impurities present in low molecular weight
HDPE from the manufacturing process.37 These aromatic ketones attach to the HgI2 surfaces by weak
Van der Waals bonds and inhibit growth on the {110} faces. When tested with purified ketones instead of
polyethylene, such as 3-hexadecanone or 14-heptacosanone, improved results were observed and near perfect
spectroscopic-grade tetragonal prismatic crystals were produced [Ariesanti and McGregor 2017]. Still the
resulting crystals are only a few mm3 to 1 cm3 in volume.
HgI2 detectors have fewer commercial applications than CdTe or CdZnTe detectors, mainly because of
process and fabrication issues. Slicing and sectioning of a layered crystal like HgI2 is difficult, often leading
to delamination and mechanical damage. To reduce damage, sectioning is often performed with a chemical
string saw, usually soaked with KI solution. A KI solution etch is usually used to remove surface damage after
the crystal is reduced to the proper size and shape. HgI2 is also highly reactive and only a few materials are
known to be compatible for electrical contacts, those being carbon (Aquadag R
), Pd, and Pt. HgI2 detectors
are usually encapsulated with parylene to prevent decomposition over time. Also, the material is known to
polarize and is manifested as a gradual change in spectral features over time.
HgI2 detectors are mostly fabricated as planar detectors, but because of the relatively low hole mobility,
significant hole trapping can occur for thick detectors. Such an effect is shown by the lower energy tail in the
spectrum of Fig. 16.56. Alternative detector designs with weighting potentials emphasizing electron charge
induction have improved energy resolution, with some success realized with pixelated imaging detectors
[Patt et al. 1995, 1996, 1997; Zhu et al. 2007]. The Frisch collar design has also been used with good results
(see Fig. 16.57), evidently showing no signs of polarization [Ariesanti et al. 2010, 2011]. During the 1980s,
HgI2 was also explored as the photodetector for scintillators having relatively longer wavelengths [Markakis
1988a, 1988b]. Unfortunately, gamma-ray events were also directly detected in the HgI2 photodetector,
which added to the background. This effect was reduced by limiting the thickness of HgI2 photodetectors to
only 2 mm. One such device, when coupled to a 2.54-cm diameter × 2.54-cm-thick block of CsI:Tl, yielded
room-temperature energy resolution of 5% FWHM at 662 keV [Markakis 1988b]. A modestly successful
application of HgI2 was as x-ray spectrometers for analysis of lead paint [Wang et al. 1993], and was offered

37 Crystalimprovement is observed only with low molecular weight polyethylene. Addition of high-purity spectroscopic grade
polyethylene or HDPE does not produce any observed change in the crystal quality.
790 Semiconductor Detectors Chap. 16

commercially for many years.38 These small detectors proved efficient for low energy gamma rays and x
rays and had excellent room temperature energy resolution (see Fig. 16.56, for example). Individual HgI2
detectors have been offered as commercial units from time to time, but presently are relatively difficult to
acquire.

Thallium Bromide (TlBr)


Thallium bromide (TlBr) is a wide band-gap semiconductor that is also of interest as a room-temperature
gamma-ray spectrometer. TlBr is a yellowish-green transparent crystal with a 2.68 eV indirect band-gap
energy. The crystal forms as a body centered cubic39 with a density of 7.56 g cm−1 . The high Z components
(Z = 81/35) make it especially attractive for gamma-ray detection. TlBr has an average ionization energy
of 6.5 eV per e-h pair, relatively large by comparison to other semiconductors used for radiation detection.
With s /0 = 29.8, the dielectric constant is also high by comparison to most semiconductors. Consequently,
the high dielectric constant increases detector capacitance, and combined with the higher ionization energy
reduces the output voltage signal by comparison to traditional semiconductors (such as Si or Ge) of similar
dimensions. With such a wide band gap, the expected intrinsic resistivity is about 1012 Ω cm, although, in
practice, TlBr usually has resistivities between 1010 and 1011 Ω cm. The electron mobility is only 6 cm2 V−1
s−1 . Mean free drift times vary with crystal quality, and electron μτ products as high as 6.5 × 10−3 cm2
V−1 s−1 along with the hole μτ products of 4 × 10−4 cm2 V−1 s−1 have been reported for highly purified
material [Shorohov et al. 2009b; Churilov et al. 2010; Kim et al. 2011; Dönmez et al. 2012] and indicates that
high quality TlBr has relatively long charge carrier mean free drift times. Although these μτ values allow
relatively efficient charge carrier collection, the low charge carrier mobilities require longer electronic shaping
times to reduce the ballistic deficit. TlBr has a melting point of 460◦ C, making it attractive for traditional
melt growth. Several melt growth techniques have been successfully used to produce quality TlBr ingots [for
example, Gostilo et al. 2003; Kozlov et al. 2004; Hitomi et al. 2007b; Zhou et al. 2009; Churilov et al. 2010].
Detector fabrication requires careful handling, mainly because TlBr is a soft crystal with a Knoop hardness
of 11.9 (approximately 1.38 on the Mohs scale) and is easily damaged.
TlBr was one of the first semiconductors explored as a radiation detector, having been investigated by
Hofstadter in 1947 [see also Hofstadter 1949a, 1949b, 1950]. Hofstadter reported that the detectors made
during these early investigations were sensitive to radiation, but failed to produce acceptable spectroscopic
results. Many years passed after these initial investigations, but TlBr was revisited by Ijaz-Ur-Rahman and
Hofstadter starting in 1984 [also Ijaz-Ur-Rahman et al. 1987]. Although these investigations yielded better
results than before, they still produced poor energy resolution and also showed polarization when operated
at room temperature. From the time of these early studies, much effort has been expended to purify TlBr
materials and study the polarization effect.
Several reports indicate that cooling of TlBr detectors seems to improve performance. Ijaz-Ur-Rahman
and Hofstadter [1984] note that the polarization effect seemed to become negligible when the detectors were
operated at a temperature of 253 K. At even lower temperatures (183 K), alpha particle energy resolution
was reported to improve, but still remained relatively poor and comparable to “a crude CsI(Tl) scintillation
counter,” although gamma-ray contributions to the spectra were non-existent. Shortly thereafter, Shah et
al. [1989, 1990] reported improved results from zone-refined material with the appearance of gamma-ray
spectra, especially at a reduced temperature (213 K). Elshazly et al. [2010] report that the mean free drift

38 Offered by TN Technologies KayRay Sensall, Inc., or TN/KSI, for many years, these XRF analyzers used small platelet grown
HgI2 detectors. The TN/KSI name was later changed to Thermo MeasureTech, a subdivision of Thermo Fisher, who no longer
produces this device.
39 By placing Tl-Br pairs at each lattice site, this crystal qualifies as a simple cubic structure. The BCC structure comes from

one constituent atom centered between eight of the other constituent atoms, where the eight other constituents populate the
corners of a cube. Each unit cell has two atoms, the usual number for BCC. The Pearson notation for the crystal is cP2.
Sec. 16.5. Compound Semiconductor Detectors 791

times increase as the temperature is lowered, especially below 160 K, and hypothesize that the notable
change may be due to a low temperature phase change.40
Purification of the TlBr material can be conducted directly with the compound, and has been shown
to make a significant difference in detector performance. Hitomi et al. [2007b] show that zone refinement
improves the carrier transport properties and has little effect on the resistivity. Energy resolution was shown
to improve for 410-micron-thick planar detectors as the number of zone refinement passes increased. For
example, energy resolution improved from 33% FWHM to 11% FWHM for 59.5-keV gamma rays when the
refinement passes were increased from 1 to 300. Gostilo et al. [2003] studied the effect of the growth method
on performance, mainly as a comparison between Stockbarger and traveling molten zone (TMZ) methods,
and concluded that the results were comparable. However, hole transport was observed to improve with the
TMZ method while electron transport improved with the Stockbarger method.
TlBr detectors are most commonly constructed as planar detectors. The general process includes slicing
wafers from an ingot with a precision wire saw followed by mechanical polishing and surface etching. Ex-
amples include Owens et al. [2003a]; Vaitkus et al. [2004]; Hitomi et al. [2009]; and Churilov et al. [2010].
Diamond wire saws and SiC slurry wire saws have both been used for the slicing process. Polishing with
Al2 O3 slurries are the most common, although diamond pastes have also been used. The mechanical polish
is often followed by an etch in 5% bromine/methanol solution. The reported final detector thicknesses are
usually between 200- to 400-microns thick in most cases. Contact patterns are applied through a shadow
mask, and have been fabricated from a variety of metals, including Au, Cr, Tl, Pt, and colloidal carbon,
as well as layered structures such as Cr/Au and Tl/Al. Thin Pd wires are often bonded to the conductive
contacts with colloidal carbon solutions. Detectors fabricated with a pixel array were processed in the same
manner as above, with the exception that the pixel side of the device was patterned with a pixelated shadow
mask, while the other was coated as with a common planar detector [Owens et al. 2003c; Hitomi et al. 2007].
Planar detector designs are susceptible to resolution degradation from charge carrier losses, primarily hole
trapping, yet have yielded in some cases an energy resolution at room temperature of about 2.2% FWHM at
662 keV for thin devices (nominally 2 mm) [Shorohov et al. 2009a]. Improved performance is achieved with
alternative designs using electron-dominated weighting potentials and in some cases electronic corrections.
By using the Frisch collar design of McGregor [2004], energy resolution for planar detectors was improved
by Kim et al. [2012], and achieved a room temperature energy resolution of 2.4% FWHM at 662 keV for
8.4-mm long TlBr detectors. In that same work, using the depth correction method of He et al. [1996], a
13-mm-thick array, having 25 pixels each 2 mm × 2 mm, achieved 2% FWHM energy resolution for 662-keV
gamma rays at a temperature of 255 K. Room temperature energy resolution of 2% FWHM at 662 keV was
achieved with a combination of depth correction and pulse height rejection for a pixel array 1.8-mm thick
[Hitomi et al. 2007a]. In recent times (as of this writing), most TlBr detectors are fabricated as pixelated
arrays to take advantage of the small pixel effect. Usually one or more pixels outperform the other pixels,
an indication of remaining problems with material or contact uniformity. Regardless, energy resolution of
about 1.5% FWHM was reported for some pixels on these TlBr detectors [Kim et al. 2009; Churilov et al.
2010].
TlBr has a serious problem with destructive polarization when operated over extended periods of time.
As noted originally by Ijaz-Ur-Rahman and Hofstadter [1984], the polarization issue was rendered negligible
when detectors were operated at temperatures below 253 K. Studies by Vaitkus et al. [2005] on Au contacted
TlBr detectors provide evidence that polarization is caused by the drifting of Tl+ ions through the TlBr

40 Notably, TlBr grown as thin films reportedly has a phase change at low temperatures, from the usual body-centered cubic
lattice (such as CsCl) at room temperature to either an orthorhombic or NaCl cubic phase [Schulz 1951; Blackman and Khan
1961]. Because these earlier measurements were conducted on thin TlBr films, and that thicker films appear to lack this
property, Smith [2013] concludes that a bulk phase change is unlikely. Regardless, there appears to be no additional evidence
that a phase change is responsible for the improved performance.
792 Semiconductor Detectors Chap. 16

crystal. Datta and Motakef [2015] observed migration and ionic conduction from Tl+ ions and Br− ions
through TlBr detectors fabricated with thin Au contacts. Using optical transmission, Datta and Motakef
[2015] recorded the progression of defect formation across a detector over several hundred hours and found
that the defects nucleate at the cathode surface and propagate to the anode. From calculations on the
formation of native defects in TlBr, Du [2010] produced three important observations. First, the native
defects have low formation energies and do not produce electron traps and, thus, can explain the relatively
large μτ products. Second, the resistivity of the material is not caused by traditional deep level compensation,
but instead by paired defects that do not induce the formation of deep traps. These defects are nearly
stoichiometric TlBr and are mainly Schottky defects that pin the Fermi level near midgap. Third, the
material has low diffusion barriers to several native defects, thereby enabling ionic conduction. It is this ionic
conduction that can cause the appearance of polarization as these native defects drift through the material,
as proposed earlier by Vaitkus et al. [2004, 2005]. Along with these polarization mechanisms generally
observed with high-quality TlBr, Du [2010] recommends that temperature reduction can reduce this ionic
conduction (already observed by Ijaz-Ur-Rahman and Hofstadter [1984]), and the use of Tl electrodes to
neutralize the diffusing (drifting) defects (as observed by Hitomi et al. [2008, 2009]). Kozorezov et al. [2010]
report the observation of polarization of TlBr with x rays of energies greater than 50 keV, manifested by a
gradual degradation of the detector charge collection efficiency. Consequently, spectroscopic features were
also observed to degrade over time. Kozerezov et al. [2010] conclude that the radiation induced polarization
is caused by hole trapping and the resultant space charge buildup. Hitomi et al. [2008] studied various metal
layered contacts with combinations of Au and Tl. Evidently, long-term operation has been successful with Tl
contacts, for which Hitomi et al. [2009] report 600 hours of room-temperature operation without observing
the polarization effect. Datta and Motakef [2015] also report improved results with Pt contacts, although
measurements still indicated degradation of the Pt contact with time [Motakef and Datta 2015; Datta and
Motakef 2015]. TlBr detectors presently remain mainly experimental devices, although some commercial
vendors are offering detectors on a custom order basis.

Lead Iodide (PbI2 )


The properties of lead iodide (PbI2 ) indicate that it is a promising material for use as a room-temperature
radiation detector. It has periodically been investigated as a potential room-temperature operated detector
since the initial investigations by Roth and Willig [1971]. PbI2 has a hexagonal close-pack (HCP) crystal
structure and a mass density of 6.16 g cm−3 . The dielectric constant reportedly ranges between 4.3 and
5.2 [Glasser et al. 1967]. The band-gap energy is reportedly between 2.3 eV and 2.55 eV. The relatively
large band-gap energy leads to low leakage currents even at elevated temperatures. The reported charge
carrier mobilities are 8 cm2 V−1 s−1 for electrons and 2 cm2 V−1 s−1 for holes [Manfredotti et al. 1977].
Unfortunately, these low mobilities, coupled with short mean free drift times, produce small μτ products,
the largest measured at μe τe = 1 × 10−5 cm2 V−1 and μh τh = 3 × 10−7 cm2 V−1 [Lund et al. 1992]. Deich
and Roth [1996] report similar μτ values of μe τe = 0.8 × 10−6 cm2 V−1 and μh τh = 6.4 × 10−7 cm2 V−1 .
Unlike HgI2 , PbI2 does not suffer from a destructive phase change at lower temperatures below the
melting temperature of 402◦ C. Hence, PbI2 can be grown directly from the melt. The high mass density
coupled with the high atomic numbers (ZI = 53, ZP b = 82) ensure a relatively high gamma-ray interaction
efficiency, similar to that of HgI2 . Initial results from research on PbI2 detectors indicated that the mean
free drift times of the charge carriers are short, and spectra obtained with this material have satellite energy
peaks for alpha particles. However, zone refinement purification of the PbI2 starting material reportedly
improved radiation spectrometer performance [Lund et al. 1988, 1992; Oliveira et al. 2002]. Detectors have
been fabricated by various methods, and samples are generally cleaved with a fine blade or sliced with a
string saw. Detector contacts have been fabricated from Au, Pd, and colloidal graphite (Aquadag R
) and
all have yielded similar results. The measured mean free drift times are 1.0 μs for electrons and 0.3 μs
Sec. 16.6. Additional Semiconductors of Interest 793

for holes. A reported room-temperature energy resolution for a 107-μm-thick device is 712 eV FWHM for
5.9-keV gamma rays and 1.83 keV FWHM for 59.5-keV gamma rays [Deich and Roth 1996]. PbI2 detectors
and materials remain experimental and are not commercially available.

16.6 Additional Semiconductors of Interest


There are a multitude of additional compound semiconductors that have been investigated as radiation
detectors, many listed in review articles describing special applications and results [Hofstadter 1949a, 1949b;
Chynoweth 1952; Mayer 1966; Swierkowski 1976, Yee et al. 1976, Armantrout et al. 1977, Sakai 1982;
Cuzin 1987; McGregor and Hermon 1997; and Owens and Peacock 2004]. Unfortunately, space limitations
preclude any lengthy discussion of all these potential alternative semiconductors that could be used for
radiation detectors. Here only three are briefly reviewed. The reader is referred to the referenced works for
more information about other semiconductor materials.
Cd1−x Mnx Te
Related to CdZnTe is the ternary compound CdMnTe, a magneto-optical material with a large Verdet
constant.41 This material is used for Faraday rotation devices, LEDs, spintronics, electro-magnetic interfer-
ence free devices, field tunable phase shifters, small coupled solar cells, phased array radar, and harsh envi-
ronment sensors [International 2017]. The band-gap dependence on elemental composition of Cd1−x Mnx Te
was studied by numerous research groups [Gaj et al. 1978; Bottka et al. 1981; Abreu et al. 1981; Diouri et al.
1982; Lemasson et al. 1983; Lee et al. 1984; El Amrani et al. 1983; Bücker et al. 1985], all of which reported a
direct band gap with a linear energy dependence on Mn concentration between 0.0 ≤ x ≤ 0.7. The band-gap
energy of Cd1−x Mnx Te at 300 K is generally described by [from data of Lee and Ramdas 1984]

Eg (x) eV = 1.524 + 1.328x eV, 0.0 ≤ x ≤ 0.7. (16.88)

The band gap can be expanded to 1.6 eV, the same as Cd0.85 Zn0.15 Te, by using x = 0.057, or
Cd0.943 Mn0.057 Te, thereby permitting room-temperature operation. The theoretical resistivity of such ma-
terial should be high enough so that injecting contacts can be used rather than blocking contacts as are
needed for CdTe:Cl.
Non-uniformities of Mn concentration causes variances in the band-gap energy and, consequently, also
increases the variance in the average ionization energy; hence uniformity is important. The segregation
coefficient (k) of Mn in a solution of CdTe is almost 1.0 so that Mn does not segregate during the growth
process. For example, Triboulet et al. [1990] report a Mn concentration gradient of only 0.48 to 0.52, when
x is 0.5 over a crystal length of 8 cm. The potential uniformity of CdMnTe is a clear benefit over CdZnTe,
for which the segregation coefficient (k) of Zn in a CdTe solution is reportedly 1.35 [Tanaka et al. 1989], so
that it is difficult to grow homogeneous CdZnTe crystals.
Triboulet et al. [1990] report that Cd1−x Mnx Te forms as a cubic zincblende crystal for x less than 0.75.
However, the crystal structure of MnTe is hexagonal, and consequently there is an increased probability
of having mixed crystalline structures between cubic zincblende and hexagonal as the Mn concentration
is increased in Cd1−x Mnx Te, especially for x greater than 0.75 for which mixed phases have been shown
to appear [Triboulet and Didier 1981]. Further, it is possible to produce hexagonal inclusions within an
otherwise cubic lattice system [Mycielski et al. 2005]. Also Triboulet and Didier [1981] report the appearance
of cubic MnTe2 precipitates within Bridgman grown crystals, and Triboulet et al. [1990] report the appearance
of twinning for Mn concentrations exceeding 15%. However, they also report that both problems can be
reduced by subsequently regrowing the ingot by the traveling heater method. From Eq. (16.88) small amounts

41 The Verdet constant describes the strength of the Faraday effect, a phenomenon in which the plane of light polarization is
rotated linearly proportional to the magnetic field in the direction of light propagation.
794 Semiconductor Detectors Chap. 16

of Mn greatly affect band-gap changes, reportedly 13 meV [Lee and Ramdas 1984] per atomic percent of
Mn,42 an indication that relatively low concentrations of Mn are required to produce high resistivity material.
Similar to CdZnTe, the formation of Cd vacancies (VCd ) produces intrinsic acceptor centers, usually
rendering as-grown material p-type with a resistivity of about 103 Ω cm. The resistivity can be increased
by annealing the ingot in Cd vapor, thereby reducing the concentration of VCd . The resistivity can also be
increased by including one or more compensating deep donor dopants into the crystal, including V [Burger
et al. 1999] and In [Kim et al. 2009]. Owens [2012] notes an additional problem with CdMnTe production
is the relatively high reactivity of Mn, which tends to bond with oxides on the growth ampoule surface, as
reported by Triboulet and Didier [1981].
The first reported use of CdMnTe for radiation detectors was by Burger et al. [1999], with x equal to
either 0.15 or 0.45, and with vanadium added as a compensation dopant. All materials studied reached
resistivities exceeding 5 × 1010 Ω cm. Spectroscopic results for detectors fabricated from Cd0.55 Mn0.45 Te
were relatively poor, but the work did show that CdMnTe has promise as a radiation detector material. Since
the time of that initial work, there has been some, but limited, pursuit of CdMnTe as a radiation detector
[Parkin et al. 2007; Zhang et al. 2007; Babalola et al. 2009; Kim at al. 2009; Rafiei et al. 2012, 2013].
Planar detectors fabricated from Cd1−x Mnx Te by Kim at al. [2009], with measured values of x between
0.074 and 0.078, had resistivities greater than 1.5 × 1010 Ω cm and μe τe of 10−3 cm2 V−1 . However,
spectroscopic measurements from low energy gamma rays delivered non-uniform results, with the best being
approximately 1.8 keV FWHM (3%) for 59.54-keV gamma rays. By employing the Frisch collar design
[see McGregor and Rojeski 2001; McGregor 2004], Kim et al. [2015] produced a 6 mm × 6 mm × 12 mm
detector from CdMnTe that yielded a room temperature energy resolution of 13.9 keV FWHM at 662 keV,
the best results reported as of this writing. CdMnTe indeed shows promise as an alternative material for
room-temperature operated semiconductor gamma-ray spectrometers, but material improvements are still
required before commercial detectors are expected to appear.
CdSe
Cadmium selenide (CdSe) has been studied as a possible room-temperature (RT) gamma-ray and x-ray
detector periodically over the last several decades [for example Burger et al. 1983; Roth 1989; Chen et al.
1998]. CdSe has atomic numbers of 48/34 with a mass density of 5.8 g cm−3 . The crystalline structure of
CdSe is wurtzite, a type of hexagonal crystal, and the band-gap energy of CdSe is 1.73 eV. Canali et al.
[1972] measured the electron and hole mobilities of CdSe, reporting μe = 720 cm2 V−1 s−1 and μh = 75 cm2
V−1 s−1 (the direction was not specified).
CdSe was first identified as a potential RT operated radiation detector by Prince and Polishuk [1967],
although it was also recognized that impurity reduction and pn junction formation were major obstacles.
A theoretical study explored the use of compound semiconductors, including CdSe, as room temperature
radiation detectors [Armantrout et al. 1977]. However, Armantrout et al. were not optimistic about CdSe
and proposed that AlSb,43 InP, ZnTe, and CdTe would be better detector candidates.
Burger et al. [1983] were first to report results for CdSe nuclear detectors. These crystals were grown
with a vertical unseeded vapor growth technique (VUVG). Typically, this crystal growth method produces
n-type material with a low resistivity ranging between 1 and 10 Ω cm [Roth 1989] and is a consequence
of Se depletion in the crystals. These samples of 250-micron thickness were heat treated at 900◦C in a Se
environment, resulting in a resistivity increase up to 1012 Ω cm, high enough to reduce leakage current for
radiation detectors. The samples were polished and etched with bromine based solutions, and subsequently
detectors were fabricated by applying Au contacts (non-symmetric) to both sides of the planar samples.

42 By comparison, the band gap of Cd1−x Znx Te increases at 6.7 meV per atomic percent of Zn.
43 Although studied often, AlSb has not developed into a commercial semiconductor for radiation detection, mainly because of
the multiple problems with the material, including the rapid decomposition of AlSb in air.
Sec. 16.6. Additional Semiconductors of Interest 795

The energy resolution of the samples when irradiated with 59.54-keV gamma rays from 241 Am was poor (or
nonexistent). Roth [1989] notes that Se treatment can produce compositional and resistivity inhomogeneities,
thereby adversely affecting charge transport properties and probably contributed to the poor resolution
performance. Notably, the samples showed temporal stability and no signs of polarization.
Burger and Roth [1984a] and Roth and Burger [1986] improved the performance of CdSe detectors by
growing crystals in a Se solution with the temperature gradient solution zoning (TGSZ) method, a technique
originally developed by Steininger [1968]. The TGSZ growth method resulted in crystals with resistivities
between 107 and 108 Ω cm. Samples ranging from 200 μm to 1.0 mm thick were prepared by cleaving or
slicing the crystals along the [12̄11] planes and subsequently etching in a bromine-methanol solution, slowly
diluted with methanol to prevent the formation of a CdBr2 layer on the surface [Roth and Burger 1986].
Contacts were formed with a carbon Aquadag R
colloidal solution. Results reported by Roth et al. [1987]
and Roth [1989] gave μe τe = 1.2 × 10 cm V−1 and μh τh ≈ 7 × 10−7 cm2 V−1 for μτ products.44 With
−5 2

these various changes and improvements (crystal growth, surface preparation, electrical contacts), improved
performance was realized, yielding 1.4 keV FWHM at 5.9 keV (55 Fe), 4 keV FWHM at 27.4 keV (125 I), and
8.5 keV FWHM at 59.54 keV (241 Am).
Chen et al. [1998] reported on CdSe detectors fabricated from commercially produced CdSe crystals with
resistivity of 1010 Ω cm. The detectors were nominally 4 mm × 4 mm area. The process used to fabricate the
devices seemed to return to the earliest detector fabrication methods and employed mechanical polishing with
alumina abrasive followed by a 2-minute etch in a 5% bromine-methanol solution. Final sample thicknesses
ranged from 150 μm to 1.2 mm, and Au contacts were applied to opposite detector sides by physical vapor
deposition. The detectors were exposed to 59.54-keV gamma rays, and produced an energy resolution of
18 keV FWHM for 150 μm thick detectors, 25 keV FWHM for 300 μm thick detectors, and no discernible
resolution for the 1.2-mm-thick detectors.
Ternary compounds such as CdZnSe [Burger and Roth 1984b; Burger et al. 1985] and CdTeSe [Fiederle
et al. 1994; Kim et al. 2008] have been explored as alternative semiconductors for radiation detection. Recall
that CdSe is a hexagonal crystal, it is interesting to note that the crystal structures of both ZnSe and CdTe
are cubic (zincblende). Hence, the varied concentrations of Se and Zn, or Se and Te, can cause not only
band-gap changes, but also crystal structural changes. Burger et al. [1985] report that the leakage current
from a Cd0.7 Zn0.3 Se sample, a wurtzite structure, was approximately an order of magnitude lower than that
of a CdSe detector of comparable size. However, the spectroscopic results were similar to CdSe reported by
Roth [1989], having 1.8 keV FWHM at 5.9 keV (55 Fe) and 4 keV FWHM at 27.4 keV (125 I). Fiederle et
al. [1994] reported on detectors fabricated from CdTe0.9 Se0.1 , a cubic zincblende crystal. Devices 1.34 mm
thick yielded 6 keV FWHM for 59.54-keV gamma rays. Kim et al. [2008] also describe the performance of
p-type Cl compensated CdTeSe, which had reported resistivity of 4.5 × 109 Ω cm. The measured charge
carrier mobilities were μe = 59 cm2 V−1 s−1 and μh = 33 cm2 V−1 s−1 , yet the reported μτ products were
high, reported to be μe τe = 6.55 × 10−2 cm2 V−1 and μh τh = 8.12 × 10−2 cm2 V−1 . However, despite these
seemingly beneficial properties, the detectors had high leakage current and performed marginally with an
energy resolution of 18 keV FWHM for 59.54-keV gamma rays.
There has been limited investigation of this wide band-gap semiconductor in recent years, perhaps due
in part to the success of other compound semiconductors such as CdZnTe. Regardless, CdSe has enjoyed re-
newed success as a nanomaterial for quantum dot fabrication. Apparently accurate control over the quantum
dot size is achievable, thereby allowing the band gap to be tailored with great precision. Potential alter-
native uses include highly efficient lasers and light emitting diodes, quantum computing, and photovoltaic

44 Chenet al. [1998] report much different values from various sources, listing μe τe = 6.3 × 10−5 cm2 V−1 and μh τh = 7.5 × 10−5
cm2 V−1 .
796 Semiconductor Detectors Chap. 16

applications through multiple exciton generation, an improvement over conventional Si solar panels [Colvin
et al. 1994; Robel et al. 2006; Somers et al. 2007].

GaSe
Gallium selenide (GaSe) was investigated as a possible room temperature radiation detector several decades
ago [for example, Manfredotti et al. 1974a; Mancini et al. 1976; Sakai et al. 1988; Nakatani et al. 1989],
although in recent years interest appears to have subsided. GaSe has atomic numbers of 31/34 with a mass
density of 4.55 g cm−3 . The crystal is hexagonal with covalently bonded Se-Ga-Ga-Se layers held together by
van der Waals bonds. GaSe has a direct band gap of 2.03 eV, wide enough for room-temperature operation.
The motivation of pursuing GaSe as a radiation detector included the search for materials capable of operating
at elevated temperatures, low cost fabrication, and minimal leakage current, all of which GaSe seemed to
possess [Manfredotti et al. 1974a; Castellano 1986].
Manfredotti et al. [1974a] communicate two methods used to produce the GaSe crystals, namely Bridgman
growth [Cardetta et al. 1972a] and a chemical transport method [Cardetta et al. 1972b]. The Bridgman
growth produced sizeable crystals of about 1 cm2 × 4 cm length with resistivities ranging between 103 to
106 Ω cm [Manfredotti et al. 1974a, 1974b]. The reported charge carrier mobilities were μe = 60 cm2 V−1
s−1 and μh = 215 cm2 V−1 s−1 measured along the c axis. The μτ products were about μe τe = 1.4 × 10−6
cm2 V−1 and μh τh = 3.65 × 10−6 cm2 V−1 , thereby indicating mean free drift times of τe = 2 × 10−6 s and
τh = 5×10−6 s. Current-voltage tests produced space charge limited characteristics as described by Lampert
and Mark [1970]. Samples grown by chemical transport were smaller in size, the largest being about 50 mm2
area and 150 μm thick and had substantially higher resistivities between 108 to 109 Ω cm. However, the
reported transport properties were inferior to the Bridgman samples, with μe τe = 1.3×10−7 cm2 V−1 yielding
τe ≈ 2 × 10−9 (results for holes were not reported). Detectors were fabricated by evaporating 7 mm2 area
Au contacts onto opposite sides of planar samples ranging between 50 to 120 μm thick. Measurements with
these detectors yielded a poor energy resolution of 1.13 MeV FWHM for 5.486 MeV alpha particles, along
with the observation of satellite peaks, an indication of inhomogeneous electrical properties [Manfredotti et
al. 1974a]. By collimating the alpha particles to a 0.8 mm2 area on the detector the energy resolution was
improved to 370 keV FWHM.
Sakai et al. [1988] and Nakatani et al. [1989] report on Bridgman grown GaSe material with measured
charge carrier mobilities of μe = 70 cm2 V−1 s−1 and μh = 45 cm2 V−1 s−1 . The average ionization energy
was found to be between 4.0 and 4.5 eV per e-h pair, and falls on the alternate dependence of the Klein
model (see Fig. 16.2), like many other layered semiconductors (HgI2 , PbI2 ). The best RT energy resolution
reported by Sakai et al. [1988] and Nakatani et al. [1989] was approximately 250 keV FWHM for 5.486 MeV
alpha particles. Yamazaki et al. [1993] experimented with GaSe doping of various elements, primarily Si,
Ge, and Sn, a doping which decreased the leakage currents. Spectroscopic measurements with these doped
samples yielded varied energy resolution, ranging from 220 keV (4%) FWHM to 850 keV FWHM for 5.486
MeV alpha particles. Yamakazi et al. [1993] also report that the best of the undoped GaSe detectors they
fabricated yielded an energy resolution of 252 keV (4.6%) FWHM for 5.846 MeV alpha particles. Most of
the undoped GaSe samples generally produced leakage current too high to yield spectroscopic results.
GaSe has also been explored for x-ray and low energy gamma-ray detection [Castellano 1986; Arutyunyan
et al. 1989; Mandal et al. 2007], and also as muon beam monitors [Manfredotti et al. 1975; Mancini et al.
1976]. Castellano [1986] and Arutyunyan et al. [1989] studied GaSe as an x-ray beam dose monitors, and
reported primarily on the photocurrent produced by x-ray beams. Castellano [1986] promoted the concept
of using GaSe for x-ray dosimetry because of its apparent thermal stability, low dark current, and simplistic
detector construction. Mandal et al. [2007] report on the spectroscopic performance of In-doped Bridgman
grown GaSe exposed to 59.54-keV gamma-rays, yielding 2.4 keV (4%) FWHM.
Sec. 16.7. Summary 797

Problems that exacerbate the progress of GaSe as a radiation detector include the fragility of the crystals,
relatively low charge carrier mobilities, and the resultant relatively low μτ products. The crystals are soft
(Mohs hardness of 2) and usually separate or cleave along the van der Waals bonds, thereby making slicing
and detector fabrication challenging. The addition of In as a dopant appears to have a positive effect on
strengthening the crystal structure [Voevodin et al. 2004]. Improvements with purification and crystal growth
may increase charge carrier mean free drift times and result in higher μτ products; however, the direct band
gap indicates relatively short charge carrier lifetimes still persist. The charge carrier mobilities are intrinsic
properties, thereby meaningful improvements are not expected.
The layered structure of GaSe produces highly anisotropic electrical properties that are beneficial for
non-linear optics [Brebner 1964]. Non-linear GaSe optical materials are used in the frequency conversion
of laser light, which involves shifting the wavelength of monochromatic laser light to alternate wavelengths
[Kübler et al. 2005], and has been exploited recently for THz generation with an extremely large bandwidth
of up to 41 THz [Huber et al. 2000; Liu et al. 2004]. GaSe is one of the most widely employed crystals
for non-linear optical generation and detection of THz radiation. Consequently small GaSe crystals are
commercially available, but primarily with common sizes about 1 cm2 × 200 μm to 1 mm thick.

16.7 Summary
Semiconductor materials are attractive as radiation detectors for two principle reasons. First, because of
their low average ionization energy w, semiconductors produce a large number of signal charge carriers per
unit energy, thereby decreasing statistical fluctuations beyond that of gas-filled and scintillation detectors
and, as a consequence, produce a much better energy resolution. Second, semiconductor materials have
energy band structures that allow their electrical properties to be altered through the addition of impurities.
These materials can be manipulated to have a majority of negative (n-type) electrical charge carriers, or
electrons, or positive (p-type) charge carriers, denoted as “holes”. Adjacent n-type and p-type materials can
be manipulated to form detectors with rectifying contacts, in which both leakage current and electrical noise
are reduced.
Moreover, semiconductor detectors can be fashioned into various types of detectors especially designed
for x-ray detection, γ-ray detection, or charged-particle detection. Detector performance is optimized by
semiconductor choice and device design. Charged-particle detectors are generally designed with low Z
material, such as Si, to reduce backscattering. Higher Z materials, because of their improved absorption
efficiencies, are generally used for γ-ray detectors. Low energy x-ray and γ-ray detectors are often fabricated
from Li-drifted Si (Si(Li) detectors), although the most commonly used semiconductor for photon detection
is high-purity Ge (HPGe detectors). Both Si(Li) and HPGe detectors must be cooled to low temperature for
best operation. Wide band-gap semiconductors, such as CdZnTe, can be used as room-temperature operated
γ-ray spectrometers.
Finally, semiconductor materials can be fashioned into arrays to yield spatial interaction information.
These arrays can be arranged from the tiling of numerous individual detectors, or they can be fabricated as
pixels upon a single semiconductor substrate. Commercial vendors offer numerous varieties of semiconductor
detectors, which include particle, x-ray, and γ-ray detectors, in the form of individual devices or as arrays.

PROBLEMS
1. A 7-mm slab of π-type Si with NA = 1014 cm−3 has a layer of Li evaporated upon it. The temperature
is raised to 400◦C for 3 hours. Afterwards, the temperature is lowered to 120◦ C, and 500 volts are
applied for a period of 100 hours. What is the resulting compensated width?
2. A surface-channel CCD device is to be used to measure alpha particles from 148 Gd. The background
concentration is NA = 1012 cm−3 , the effective operating bias is 10 volts, and the oxide thickness is 0.15
798 Semiconductor Detectors Chap. 16

microns. If the pixel sizes are 5 micron × 5 micron area, what is Qmax ? Will this device operate for
the intended use?

3. A Si(Li) detector has a linearly varying residual positive space charge. Derive a general expression for
the electric field distribution in a planar detector under such a condition.

4. Determine the electron and hole velocities for a 5 mm × 5 mm × 1 cm thick CdZnTe detector operated
at 1000 volts.

5. How would a change in the Fano factor in a germanium detector affect the energy resolution of the
detector?

6. Plot your estimate of the energy resolution of a HPGe detector as a function of the incident photon
energy between 100 keV and 10 MeV. Assume that there is complete charge collection and that there
is negligible noise.

7. How thick must the depletion region in a Si(Li) be to record the full energy of a 4-MeV alpha particle?

8. You have a Si surface barrier detector with the following characteristics: n-type Si, n = 2 × 1014 n-type
dopant impurities cm−3 , and Vbi = 0.3 volts. You also have an 241 Am alpha particle source. The
detector is operated in vacuum. (a) What does the differential pulse height spectrum appear as with no
voltage on the detector? (b)What does the differential pulse height spectrum appear as with 25 volts
applied? (c) How much voltage is required to extend the detector depletion region just beyond the alpha
particle range?

9. Given a Si(Li) detector with a 3.5-mm-thick drifted region, determine the energy that the detector can
measure from an energetic electron of 20 MeV if the electron passes through the detector.

10. You measure spectra from a detector fabricated from CdTe that suffers much charge carrier trapping.
A few measurements reveal the following: electron mean free drift times are 0.5 microseconds, electron
mobility = 1000 cm2 V−1 s−1 , hole mean free drift times are 0.2 microseconds, electron mobility = 80
cm2 V−1 s−1 , and saturation velocity for both carriers is 107 cm s−1 .
The operating voltage is kept at 100 volts. (a) With highly penetrating gamma rays (high energy),
what is the maximum detector thickness that the detector can be to keep the measured pulses below
20% deviation? (b) 10% deviation? (c) 1% deviation?

11. What is the best theoretical energy resolution that you can achieve with Ge for 122-keV gamma rays
in Ge? Give answers in energy and percent. Repeat for 1.17 MeV gamma rays.

12. You are given pure Ge material with the properties: NC = 1019 cm−3 and NV = 6 × 1018 cm−3 . (a)
What is the value of ni at T = 77K? (b) What is the value of ni at T = 300K? (c) Explain why
germanium detectors are operated at cryogenic temperatures.

13. Why are escape peaks generally more prominent in spectra from HPGe detectors to those observed with
NaI:Tl detectors of equal volume?

14. What properties of a semiconductor material are of most concern to you when considering using the
material as a radiation detector? Consider both technical and practical aspects of using the material.
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Chapter 17

Slow Neutron Detectors

When a neutron enters a nucleus, the effects are about as catastrophic as if the moon struck the
earth. The nucleus is violently shaken up by the blow, especially if the collision results in the
capture of the neutron. A large increase in energy occurs and must be dissipated, and this may
happen in a variety of ways, all of them interesting.
I.I. Rabi

Neutron detection is challenging primarily because neutrons, like photons, do not have an electrical charge,
i.e., they are classified as indirectly ionizing radiation. Unlike α and β radiations, neutrons must first interact
in a medium to produce directly ionizing reaction products, or at least some other observable effect. Neutron
detectors usually rely upon an interaction with the atomic nuclei within the detector medium and most often
it is an absorption or scattering interaction. Slow neutron detectors usually incorporate neutron reactive
materials with relatively large neutron absorption cross sections in the low energy region below about 1
keV, whereas fast neutron detectors quite often have relatively large scattering cross sections for neutron
energies above 500 keV. Because the differences between the detection methods are considerable, this chapter
is devoted to slow neutron1 detectors while the next chapter discusses fast neutron detectors.
Slow neutron detectors usually rely upon reactive neutron absorptions for the detection mechanism.
Neutrons are absorbed in the target material and the resulting compound nucleus emits ionizing radiations.
Most of the neutron absorbing materials used for the neutron detection emit heavy charged particles, although
some of the less frequently used materials emit conversion electrons, beta particles, or gamma rays. The
three most popular reactive materials for slow neutron detection are 3 He, 10 B, and 6 Li while alternative
reactive materials include Gd, U, Hg, and Cd.

17.1 Cross Sections in the 1/v Region


An important characteristic of the 3 He, 10 B, and 6 Li isotopes is that they are all so-called 1/v absorbers.
Radiative capture of low-energy neutrons can be modeled with the Breit-Wigner one-level formula [Lamarsh
1966]

2 E1 Γn Γγ
σγ (Ec ) = πγ1 g , (17.1)
Ec (Ec − E1 )2 + Γ2 /4

1 Inmost instances the totality of slow neutrons are called thermal neutrons, i.e., neutrons with speeds that are in thermal
equilibrium with the thermal motion of the ambient medium through which they diffuse (see Problem 17-1). An exception
would be a beam of monoenergetic slow neutrons produced by a neutron diffractometer.

813
814 Slow Neutron Detectors Chapt. 17

where E1 is the energy of the lowest absorption resonance peak, Ec is the center-of-mass energy between
the neutron and target nucleus, γ1 is the reduced de Broglie wavelength for a neutron at energy E1 , g is a
statistical factor that is a function of the spin of the target nucleus and the resulting compound nucleus, and
Γn , Γγ , and Γ = Γn + Γγ are, respectively, the width for neutron emission, the width for the (γ, n) reaction,
and the total width of the resonance.2
The statistical factor g gives the probability that a particular compound state is formed and is given by
 
1 2J + 1
g= , I=0 (17.2)
2 2I + 1
or g = 1 if I = 0, where I and J are, respectively, the spins of the target nucleus and the compound nucleus.
The Breit-Wigner formula is derived for the center-of-mass system so that for an incident neutron of speed
v the value of γ1 is given by

γ1 = , (17.3)
μv
in which μ is the reduced mass of the nucleus-neutron system, i.e.,
Amn
μ= , (17.4)
A+1
where mn is the neutron mass and Amn is the mass of the target nucleus. For heavy nuclei A mn and
μ  mn so these center-of-mass nuances are not important; but they are for light target nuclei.
Because E1 , γ1 , Γγ , Γn , and Γ are constants in Eq. (17.1), the radiative capture cross section produces
the observed 1/vc behavior at low neutron energies (Ec  E1 ), namely

E1 K2
σγ ≈ K1 = , (17.5)
Ec vc
where K1 and K2 are proportionality constants.
Similarly, the cross section for neutron capture resulting in the release of charged particle reaction prod-
ucts can be expressed as [Lamarsh, 1966]

Eb K3
σ(a,b) = H(Ea ) ≈ , (17.6)
Ea va
for the reaction X(a, b)Y , where Ea and Eb are the kinetic energies of the particles in the center-of-mass
system and H(Ea ) is a correction factor for non-1/v behavior for moderately large Ea  E1 , and K3 is a
proportionality constant. Neutrons at low energy (Ea  E1 ) have little effect on the reaction Q value, so
the Q value of the reaction is nearly equal to Eb . In such cases, H(Ea ) ≈ 1.
Consider the laboratory system in which neutrons approach target nuclei with relative velocities

vr = v − V, (17.7)

where v is the neutron velocity vector and V is the target nuclei velocity vector in the laboratory system.
As observed from the target nuclei, the incident neutrons are a differential beam of intensity

dI = n(v)vr dv, (17.8)

2 The“width” is a measure of the probability the compound nucleus decays in a specific manner; it is equal to  times the
decay constant for the particular process.
Sec. 17.2. Slow Neutron Reactions Used for Neutron Detection 815

where n(v) is the neutron density distribution and vr = |vr |. The neutrons interact with the nuclei at a
reaction density rate
dF = n(v)N (V)σ(vr )vr dv dV (cm−3 s−1 ), (17.9)
where N (V) is the target nuclei velocity density distribution and σ(vr ) is the neutron cross section at the
relative speed vr . The total interaction rate density is then

F = n(v)N (V)σ(vr )vr dv dV. (17.10)

If the target nuclei exhibit a 1/v absorption behavior, then from Eq. (17.5) and Eq. (17.6), any arbitrary
absorption cross section σa (vro ) for relative speed vro is related to the cross section at vr by
σa (vro )vro
σa (vr ) = . (17.11)
vr
Substitution of Eq. (17.11) into Eq. (17.10) yields

Fa = n(v)N (V)σa (vr )vr dv dV


σa (vro )vro
= n(v)N (V) vr dv dV
vr

= N σa (vro )nvro = Σa (Eo )nvo , (17.12)


where Σa (Eo ) is the macroscopic reaction cross section at an arbitrary reference speed vo (most often chosen
as 2200 m/s), n is the total neutron density, and N is the total target nuclei density. The result of Eq. (17.12)
is very important and shows that the reaction rate of neutrons with a 1/v material is independent of the
neutron or target nuclei velocity distributions. Hence, a measurement using a reaction rate to determine
detection efficiency is independent of the neutron energy distribution for 1/v absorbers. Note that the result
of Eq. (17.12) is restricted to the 1/v region of the neutron cross section, generally applicable to only slow
neutrons. In the case that the absorber nuclei are non-1/v, a temperature dependent Westcott correction
factor ga (T ) is required to correct for non-1/v interaction behavior [Lamarsh 1966]
F = ga (T )Σa (E0 )nv0 , (17.13)
where T is the neutron temperature of the assumed Maxwellian spectrum of interacting thermal neutrons.

17.2 Slow Neutron Reactions Used for Neutron Detection


As previously noted, the three most popular isotopes for slow neutron detection are 3 He, 10 B, and 6 Li, all
having 1/v dependence in the slow neutron region (see Fig. 17.1). In all three cases, reactions with slow
neutrons cause the reaction products to be ejected in opposite directions (180◦ ). While 3 He is used for
gas-filled detectors, both 10 B and 6 Li are used in a variety of detector configurations, including gas-filled,
scintillator, and semiconductor devices.
There are also numerous large Z absorbers used for neutron detection that do not exhibit 1/vc behavior
because of resonances appearing in the epithermal and thermal-neutron range. Unfortunately, the interac-
tion rate for such absorbers is dependent on the neutron and target nuclei velocities. Consequently, more
information must be known about the neutron flux and energy distribution to accurately calibrate instru-
ments utilizing these absorbers than expressed by the simple expression of Eq. (17.12). Nevertheless, many
are useful for neutron detection, with some of the more important ones that have very large thermal-neutron
absorption cross sections being 113 Cd, 157 Gd, 199 Hg, and 235 U.
816 Slow Neutron Detectors Chapt. 17

Figure 17.1. Neutron absorption cross sections in barns for common 1/v
neutron detector materials. The energy is the incident neutron energy in the
center-of-mass coordinate system. Data are from [ENDFPLOT, 2015].

17.2.1 The 3 He Reaction


There are two natural isotopes of helium, namely 3 He and 4 He with natural abundances of 0.000137% and
99.999863%, respectively. The isotope 3 He has a relatively large total thermal-neutron cross section of 5320
barns at 2200 m/s,3 of which the 3 He(n,p)3 H reaction constitutes 5316 barns. By contrast the thermal-
neutron absorption cross section for 4 He is essentially zero. The microscopic thermal-neutron absorption
cross-section for 3 He decreases with increasing neutron energy, with a dependence proportional to the inverse
of the neutron speed (1/v) up to about 0.1 MeV, as shown in Fig. 17.1.
For an incident neutron with negligible kinetic energy, the 3 He(n,p)3 H reaction has the following ener-
getics:
3
He + 10 n → 3 H (0.191 MeV) + 1 H (0.573 MeV) with Q = 0.764 MeV. (17.14)
The reaction products, while emitted isotropically, are emitted opposite to each other in order to preserve
the almost zero incident momentum of the neutron.
The density of natural He gas is 0.1786 g L−1 at standard temperature and pressure (STP),4 with an
atom density of 2.686 × 1019 cm−3 . Hence, the macroscopic absorption cross section (Σa ) for pure 3 He at
STP is 0.1492 cm−1 . Most neutron detectors based on 3 He are pressurized to increase the value of Σa . A
common pressure for 3 He gas-filled neutron detectors is 2.8 atm; however, detectors with pressures ranging
from 1 atm up to 20 atm are commercially available. Because of the pressurization, various national aircraft
regulations may limit the transport of these detectors.

3 Thermal neutrons generally have a wide range of energies that are often well-described by a Maxwellian flux distribution,
which has a most probable energy of 0.0253 eV (corresponding to a speed of 2200 m/s) for a neutron temperature of 293.5 K.
In this chapter, the thermal-neutron cross section refers to the 2200 m/s cross section whose values are taken from the 2017
ENDF/B-VIII library.
4 STP is 273.15 K (0 ◦ C) and 100 kPa (0.9869 atm).
Sec. 17.2. Slow Neutron Reactions Used for Neutron Detection 817

For low energy neutrons, the neutron contributes very little to the overall reaction product energies; hence
the final energy shared by the reaction products is essentially the reaction Q value. As the neutron kinetic
energy increases, the reaction products absorb and share this additional energy, yet for energies in the slow
to epithermal region, this additional energy is usually masked by the Q value energy; hence, spectroscopic
energy information is lost. The same is true for the neutron momentum, which contributes little, thereby
causing almost all momentum to be shared between the two reaction products. Hence, for slow neutrons,
reaction product net momentum is essentially zero. If one neglects the energy and momentum of the neutron,
conservation of energy and momentum yields,

E(3 H) + E(1 H) = Q = 0.764 MeV, (17.15)

and
M (3 H)v(3 H) = M (1 H)v(1 H), (17.16)
or  
2E(3 H)M (3 H) = 2E(1 H)M (1 H). (17.17)
From Eq. (17.15) and Eq. (17.17), the reaction product energies shown in Eq. (17.14) are readily obtained.
Neutron detectors based on 3 He are generally considered a standard for neutron measurements and are
widely used in various nuclear industries. However, the natural abundance of 3 He is low. The problem
is further exacerbated by the dwindling supply of 3 H gas,5 which decays by β-particle emission into 3 He.
Liquid 3 He also has unique superfluid properties for ultra-low-temperature physics, thereby creating another
demand for this scarce resource. Consequently, 3 He gas and detectors are relatively expensive, costing
thousands of US dollars per liter at STP.

10
17.2.2 The B Neutron Reaction
There are two natural isotopes of boron, namely 10 B and 11 B with natural abundances of 19.9% and 80.1%,
respectively. The isotope 10 B has a relatively large thermal-neutron (2200 m/s) cross section of 3847 barns,
of which the 10 B(n,α)7 Li cross section constitutes 3844 barns. The microscopic thermal-neutron absorption
cross section for 10 B decreases with increasing neutron energy, with a dependence proportional to the inverse
of the neutron speed (1/v) over much of the slow energy range, as shown in Fig. 17.1. The density of natural
B is 2.35 g cm−3 , and the density of enriched 10 B is 2.16 g cm−3 . The resulting macroscopic thermal-neutron
cross section (Σa ) for natural B material is 100 cm−1 and 497 cm−1 for fully enriched 10 B material.
The 10 B(n,α)7 Li reaction leads to the following reaction energetics when the incident neutron has negli-
gible energy:
$ 7 ∗
Li (0.840 MeV) + α (1.470 MeV) Q = 2.310 MeV 94%
10
B+ 1
0n → . (17.18)
7
Li (1.015 MeV) + α (1.777 MeV) Q = 2.792 MeV 6%

The reaction products are emitted isotropically but in opposite directions when thermal neutrons (with
negligible momentum) are absorbed by 10 B. After absorption, 94% of the reactions leave the 7 Li ion in its
first excited state, which rapidly deexcites to the ground state in about 10−13 s by releasing a 480-keV
gamma ray. For a variety of neutron detectors, especially gas-filled neutron detectors, the 480-keV gamma
ray usually escapes and does not contribute to the detection output. The remaining 6% of the reactions

5 Much of the world’s 3 H came from the tritium generated for nuclear weapons production, which today has been significantly
reduced by international treaties.
818 Slow Neutron Detectors Chapt. 17

produce a 7 Li ion in its ground state. Conservation of energy and momentum then requires

E(7 Li*) + E(4 He) = Q = 2.310 MeV, (17.19)

E(7 Li) + E(4 He) = Q = 2.792 MeV, (17.20)

and
 
2E(7 Li*)M (7 Li*) = 2E(4 He)M (4 He), (17.21)
 
2E(7 Li)M (7 Li) = 2E(4 He)M (4 He). (17.22)

Simultaneous analysis of Eq. (17.19) with Eq. (17.21), and Eq. (17.20) with Eq. (17.22) yields the reaction
product energies shown in Eq. (17.18).

17.2.3 The 6 Li Neutron Reaction


There are two natural isotopes of lithium, namely 6 Li and 7 Li, with natural abundances of 7.59% and
92.41%, respectively. The isotope 6 Li has a relatively large thermal-neutron cross section of 938.8 barns
with the 6 Li(n,t)4 He reaction contributing 938.0 barns. The nuclide 7 Li has a relatively small thermal-
neutron absorption cross section of approximately 45.5 mb. The microscopic thermal-neutron absorption
cross-section of 6 Li decreases with increasing neutron energy, with a dependence proportional to the inverse
of the neutron speed (1/v) over much of the energy range, with a notable resonance near 240 keV as shown
in Fig. 17.1. The density of natural Li is 0.534 g cm−3 , and the density of enriched 6 Li is 0.463 g cm−3 . With
an atomic density of 4.65 × 1022 atoms cm−3 , the resulting macroscopic thermal neutron cross section (Σa )
for natural Li material is 3.300 cm−1 and 43.48 cm−1 for enriched 6 Li material. The 6 Li(n,t)4 He reaction
leads to the following products:
6
Li + 10 n → 4 He (2.05 MeV) + 3 H (2.73 MeV) Q = 4.78 MeV. (17.23)

Again they are emitted isotropically but in opposite directions if the incident neutron energy is sufficiently
small. Conservation of energy and momentum, for negligible incident neutron momentum, yields

E(4 He) + E(3 H) = Q = 4.78 MeV, (17.24)

and  
2E(4 He)M (4 He) = 2E(3 H)M (3 H). (17.25)
Simultaneous solutions of Eq. (17.24) with Eq. (17.25) yields the reaction product energies shown in
Eq. (17.23).
Because of its higher absorption cross section, the 10 B(n,α)7 Li reaction leads to a generally higher reaction
probability than the 6 Li(n,t)4 He reaction for neutron energies below 100 keV. However, the higher energy
reaction products emitted from the 6 Li(n,t)4 He reaction lead to greater ease of detection than do the particles
emitted from the 10 B(n,α)7 Li reaction.
Although there are neutron detectors based on enriched 6 Li metal, careful handling is required because
Li metal is highly reactive in the presence of water moisture or other oxidizers. A popular and relatively
non-reactive Li compound used for neutron detection is 6 LiF. The molecular density of 6 LiF is 6.12 × 1022
molecules cm−3 which also equals the atomic density of the 6 Li atoms.6 The mass density of 6 LiF is 2.54 g
cm−3 , which produces a macroscopic thermal-neutron (n,α) cross section of 57.41 cm−1 .

6 It is interesting to observe that the atomic density of Li atoms in LiF is actually higher than in pure Li metal.
Sec. 17.2. Slow Neutron Reactions Used for Neutron Detection 819

Figure 17.2. Neutron absorption cross sections in barns for common non-1/v
neutron detector materials, showing the radiative capture cross sections for
113 Cd, 157 Gd, and 199 Hg. For such heavy nuclide targets the center-of-mass

neutron energy almost equals the neutron energy in the laboratory system.
Data are from [ENDFPLOT, 2015].

155 157
17.2.4 The Gd and Gd Neutron Reactions
157 158
The Gd(n,γ) Gd reaction leads to the emission of low energy internal conversion electrons,
most of which are emitted at energies below 220 keV, along
with an assortment of gamma rays. The attractiveness of Table 17.1. Conversion electron energies and emis-
sion fractions for neutron interactions in natural
157
using Gd is because of its large (n,γ), thermal-neutron Gd. The conversion electrons are produced from
cross-section of 252.9 kb. 157 Gd has low-energy absorp- both 155 Gd(n,γ)156 Gd and 157 Gd(n,γ)158 Gd reactions.
tion resonance at 2.82 eV and, consequently, its micro- Data are from [Schulte et al., 1994].
scopic neutron absorption cross section does not have a Energy Electrons/ Energy Electrons/
(1/v) dependence in the sub eV range as is evident from (keV) neutron (%) (keV) neutron (%)
Fig. 17.2. Another neutron absorbing Gd isotope that 29 9.82 149 0.84
cannot be ignored is 155 Gd, which has a thermal-neutron 39 4.19 173 1.46
(n,γ) cross section of 60.74 kb. Together these two iso- 71 26.80 180 0.31
topes of Gd are perhaps the largest of the solid-state 78 6.17 191 0.30
7 81 4.97 198 0.06
thermal-neutron absorbers. The density of natural Gd
−3 155 88 1.16 228 0.40
is 7.901 g cm , and the natural abundances of Gd 131 3.41 246 0.02
and 157 Gd are 14.80% and 15.65%, respectively.
Although some of the other existing Gd isotopes have significant thermal-neutron (n,γ) cross sections,
they do not contribute to the neutron detection capability of this element. For example, 152 Gd has a 735.1
b 2200-m/s (n,γ) cross section and an abundance of 0.020% while 154 Gd has a 85.2 b cross section and a

7 The radioactive gas fission product 135 Xe has a thermal-neutron (n,γ) cross section of 2.6 Mb, the largest of any isotope.
820 Slow Neutron Detectors Chapt. 17

2.18% abundance. The three other stable isotopes 156 Gd, 158 Gd and 160 Gd have negligible cross sections of
1.80 b, 2.03 b, and 1.41 b, respectively.
Given the natural abundances of the isotopes in natural Gd, the natural Gd macroscopic thermal-neutron
absorption cross is 1467 cm−1 . This macroscopic absorption cross section could be increased by using enriched
157
Gd; however, in practice it is impractical due to the high cost of isotope separation.
Neutron absorptions in Gd produce an abundance of spontaneous internal conversion electrons and
gamma-rays from the excited 156 Gd and 158 Gd nuclei. Although the gamma-ray emissions can be used
to indicate neutron interactions, it is usually the conversion electrons that are used in the detection process.
Shown in Table 17.1 is a list of conversion electron energies and relative emissions (%) per captured neutron,
totaling only 59.91% of the product yield [Aoyama et al. 1992]. The most salient emission of conversion
electrons is that from the excited state of 158 Gd nucleus and produces an electron with an energy of 71 keV.
There are also two conversion electron emissions near 80 keV totaling 11.14% of the product yield. The total
fraction of conversion electrons above 85 keV amounts to only 7.96% of the total emissions. Hence, the lower
level discriminator must be set below 71 keV equivalent in order to detect most of the conversion electrons.
These relatively low energy conversion electrons (and accompanying gamma-ray emissions) can be difficult
to distinguish from background gamma rays in a high radiation field.

113
17.2.5 The Cd Neutron Reaction
Natural cadmium has eight existing isotopes, of which radioactive 113 Cd (T1/2 = 8.04 × 1015 y) strongly
absorbs thermal neutrons, and has a thermal-neutron (n,γ) cross section of 19.96 kb. The density of natural
Cd is 8.65 g cm−3 , and the isotope 113 Cd has a natural isotopic abundance of 12.23%. The natural Cd
macroscopic thermal-neutron absorption cross section is 113.1 cm−1 . The cross section as a function of
neutron energy is shown in Fig. 17.2. This macroscopic absorption cross section could be greatly increased
by using Cd enriched in 113 Cd, but high isotopic separation costs preclude this approach.
The 113 Cd(n,γ)113 Cd reaction produces numerous gamma-ray emissions, ranging from relatively low en-
ergies up to and beyond 9 MeV. However, there are two salient prompt gamma-ray emissions of interest
at 558.6 keV and 651.3 keV [Lone et al. 1981; Tuli 1997], with branching ratios of 72.73% and 13.9%, re-
spectively. These gamma rays can be discerned with a relatively high-resolution gamma-ray spectrometer.
Unfortunately, a gamma-ray spectrometer capable of detecting the 113 Cd(n,γ)113 Cd emissions also detects
other background gamma rays, a signal which can potentially confound interpretation of a measurement.
Also, unlike neutron reactive detector materials that emit charged-particle reaction products, neutron detec-
tors that rely on the absorption of prompt gamma-ray emissions suffer a higher signal loss because of reaction
products escaping the detector and, thus, the detection efficiency is reduced. Further, at the prompt emis-
sion energies of 558.6 keV and 651.3 keV, the most probable gamma-ray interaction in detectors is Compton
scattering, which produces a continuum of energies that can be difficult to distinguish from background
gamma rays that undergo Compton scattering in the detector and surroundings.

199
17.2.6 The Hg Neutron Reaction
The element Hg is also an interesting material for neutron detection. It has one strongly neutron reactive
isotope, 199 Hg, with a thermal-neutron (n,γ) cross section of 2150 b (see Fig. 17.2).8 The density of natural
Hg is 13.534 g cm−3 , with a 199 Hg natural abundance of 16.94%, and has a natural Hg macroscopic thermal-
neutron (n,γ) cross section of 14.80 cm−1 . As with 157 Gd and 113 Cd, enriched 199 Hg is rare and not an
economically practicable option. Hg is a toxic liquid at room temperature, which causes additional handling

8 The naturally occurring isotope 196 Hg has an even larger thermal-neutron (n,γ) cross section of 3079 b, but its small natural
abundance of 0.15% has negligible effect on the ability of Hg to absorb thermal neutrons. The five other naturally occurring
isotopes of Hg have thermal cross sections of, at most, a few barns.
Sec. 17.2. Slow Neutron Reactions Used for Neutron Detection 821

problems.9 Detectors that use 199 Hg as the neutron reactive material are usually a room temperature solid
compound or alloy of Hg.
Similar to the 113 Cd(n,γ)113 Cd reaction, there are numerous gamma-ray emissions from the
199
Hg(n,γ)200 Hg reaction; however, there is one prominent gamma-ray emission of interest at 368.1 keV
[Lone et al. 1981; Tuli 1997] with a branching ratio of 81.35%. When Hg is coupled with a high resolu-
tion gamma-ray spectrometer, the 368.1-keV energy peak can be used as a measure of neutron interactions.
Note that this prompt gamma-ray emission energy is low enough to have a reasonably high probability of
being fully absorbed in the detector, which works to improve the visibility of a full energy peak. However,
this spectral feature can still overlap with background gamma-ray spectra, thereby making measurements
difficult to analyze.

17.2.7 Fission Reactions


Fissile materials are also used as neutron detection materials, primarily in gas-filled proportional counters
named “fission chambers”. Fissile materials, such as 235 U and (rarely) 239 Pu, are also used for slow neutron
detectors (see Fig. 17.3). The fission reaction releases approximately 200 MeV of energy, approximately
150 MeV of which is transferred to the heavy charged particle reaction products. Unlike other reactions
described in this chapter, these reaction products vary, with over 100 possible reaction products emitted
after a fission reaction. However, the reaction products generally fall into a low energy branch and a high
energy branch, centered near 60 MeV and 90 MeV, respectively.

Figure 17.3. Neutron fission cross sections in barns for materials used in slow
neutron fission chambers, 235 U and 239 Pu [data are from ENDFPLOT, 2015].

The 2200 m/s thermal-neutron fission cross section for 235 U is 585.0 barns, although the fission plus
capture thermal-neutron absorption cross section is higher at 683.7 barns. The nuclide 235 U is also radioactive
with a halflife of 7.038 × 108 years, and decays by alpha-particle and gamma-ray emission. The gamma-ray
emissions have energies of 143.76 keV, 185.72 keV, and 204 keV with branching ratios of 11%, 55%, and 5%,

9 Many organic compounds of Hg are extremely toxic.


822 Slow Neutron Detectors Chapt. 17

respectively. Principal alpha particles are emitted with energies of 4.366 MeV, 4.398 MeV, and 4.58 MeV
with branching ratios of 18%, 57%, and 8%, respectively. Consequently, detectors fashioned with 235 U as
the neutron reactive converter always have an intrinsic radiation background. However, the signal produced
by the fission reaction is enormous by comparison to signals produced by the background radiations; hence
these background signals can usually be rejected by a discriminator circuit when operated in pulse mode, and
they add very little to the output current if the detector is operated in current mode. The main advantage
of using fissile materials for neutron detection is the large output signal per event that can stand out in the
midst of a high radiation background.
Slow neutron detectors based on fission reactions are usually not fabricated with highly enriched 235 U,
but instead with natural U or low enriched 235 U. Hence, a large constituent of the material is 238 U, which is
fissionable but not fissile. 238 U has a long half life of 4.468 × 109 years, and decays mainly by alpha-particle
emission with energies of 4.15 MeV (25%) and 4.20 MeV (75%). Slow neutron capture in 238 U, with a
thermal-neutron capture cross section of 2.684 barns, can transmute into 239 U (T1/2 = 23.47 minutes) which
upon beta particle decay creates 239 Np (T1/2 = 2.345 days) and upon another beta particle decay, eventually
into fissile 239 Pu. Hence, a detector with a proper mixture of 235 U and 238 U can be used to prolong the
useful detector life through neutron transmutation of 238 U into 239 Pu.
The thermal-neutron fission cross section for 239 Pu is 747.4 barns, although the total thermal-neutron
absorption cross section is slightly higher at 1017.5 barns due to a thermal-neutron capture cross section of
270.1 barns. A cross resonance at 0.295 eV yields a fission cross section of 3258 b (see Fig. 17.3). 239 Pu is
radioactive with a halflife of 2.411 × 104 years, and decays mainly by alpha-particle decay (5.105 MeV at
11% and 5.156 MeV at 88%), although there are also several gamma-ray and conversion electron emissions
with low branching ratios. Hence, an intrinsic radiation background component gradually increases with
detector use. As with 235 U, the fission products produce much larger signals than the background alpha
particle radiations, and can be easily discerned with a discriminator circuit.

17.3 Gas-Filled Slow Neutron Detectors


Gas-filled slow neutron detectors can be generally classified as one of two types: those that use neutron
reactive gases and those that use conventional proportional gases with a solid neutron reactive material
inside the detector. Grosshoeg [1979] provides a review describing the origins of these detectors. There are
two main types of neutron detectors that are backfilled with either of two neutron reactive gases, namely 3 He
gas or 10 BF3 gas. There are several variants for gas-filled detectors having internal components composed
of solid neutron reactive materials, including detectors based on 10 B, 6 Li, or 235 U materials. In all of
these detectors, slow neutrons react with the neutron absorbing material and induce currents from the
charged-particle reaction products with energies much greater than the kinetic energy of the slow neutrons.
These large reaction Q-values mask the small kinetic energies of slow neutrons and, hence, do not preserve
the original information of the neutron energy. Consequently, they cannot be used directly as neutron
spectrometers, but rather they serve as neutron counters. However, spectral features of the reaction products
do play an important role in neutron detection, mainly, the pulse height spectra allow the user to set the
discriminator at an acceptable level to remove background signals while optimizing the neutron response.

17.3.1 Detectors with Neutron Absorbing Fill Gases


The class of detectors containing neutron reactive gases all have similar energy deposition features, a con-
sequence of wall and end effects. Gas pressure and detector volume strongly affect the limiting neutron
detection efficiency in these detectors. Increased pressure generally increases the probability of absorption,
although it may also affect signal proportionality and response speed. Further, these detectors are also
Sec. 17.3. Gas-Filled Slow Neutron Detectors 823

cathode wall events


for A

Counts
D contributions
from E
anode events
events for C
A for B

E contributions
B C from D
Energy
cathode wall (MeV)
triton proton 0.191 0.573 0.764

Figure 17.4. (left) Trajectories of reaction products that cause the appearance of the wall effect. (right) Contributions
to the pulse height spectrum for the various trajectories. See the text for an explanation of the consequences.

relatively radiation hard and temperature resistant so they are able to operate at elevated temperatures and
higher neutron fluxes than other neutron detectors.
3
He Gas-Filled Detectors
3
He detectors were originally introduced in 1952 [Batchelor 1952; see also Batchelor et al. 1956] and are
presently the most popular commercially available neutron detectors. These detectors are operated in the
proportional region of the gas pulse-height curve (see Fig. 10.1). Because 3 He is a rare and expensive gas,
these detectors are not available as gas-flow proportional counters. Instead, they are generally designed
as hermetically sealed coaxial detectors. The detection method is straightforward. Neutrons enter the
gas volume and are absorbed by the 3 He to produce a compound nucleus, which spontaneously decays by
emitting two energetic charged-particle reaction products. The two reaction products pass through the
gas and produce electron-ion pairs. The electrons rapidly drift towards the anode and create a Townsend
avalanche. The drifting motion towards the cathode of the positive ion cloud from the avalanche induces
current to flow which is transformed into a voltage pulse by the attached amplification circuitry.
Wall Effect Neutron interactions can occur randomly within the 3 He detector, and in some of these
cases, the interaction occurs near the chamber cathode wall. If a reaction product strikes the wall, its
residual kinetic energy is deposited in the wall rather than the gas and does not contribute to gas ionization.
Hence, the resulting amplitude of the output pulse is reduced below that of that for a full energy deposition
event. Consequently, there are certain spectral features that are intrinsically observed from a 3 He gas-filled
detector, primarily a consequence of this wall effect.
Shown in Fig. 17.4 are various possible reaction product trajectories in a 3 He detector that form the
main wall effect features. Trajectory A represents cases in which a neutron is absorbed in the gas and both
reaction products deposit all of their initial kinetic energy in the gas volume. Reactions like type A form a
full energy peak in the pulse height spectrum. Trajectories B and C represent cases in which the neutron
is absorbed next to the cathode wall and only one of the reaction products enters the gas, while the other
reaction product deposits all of its energy in the wall. Cases B and C form the limiting minimum energy
cases for each reaction product type and produce a stairstep feature in the pulse height spectrum. Because
each reaction product has a different energy, there are two such stairstep features that appear at the triton
energy (0.573 MeV) and at the proton energy (0.191 MeV). Trajectories D and E represent those cases in
which the neutron is absorbed near the cathode wall and all of one reaction product energy is absorbed in
the gas, while only part of the other reaction product energy is absorbed in the gas before striking the wall.
Cases D and E fill in the wide range of possibilities between the limiting cases of partial energy deposition B
and C and that of full energy deposition A. Hence, cases for D and E produce a continuum of energies in the
824 Slow Neutron Detectors Chapt. 17

low field high field region low field


region region

Figure 17.5. X-ray image of a sealed 3 He gas-filled neutron detector. The detector gas
chamber is 13 cm long; however, only 8 cm of that length are in the high field region.

low field high field


region region
events
events for A
Counts

F D B for L

J events
I events for G
for F
A anode
contributions
insulator & G from J
feedthrough K contributions
L E
H C from K
Energy
cathode wall (MeV)
triton proton 0.191 0.573 0.764

Figure 17.6. (left) Reactions produce trajectories that cause the appearance of both the end effect and the wall
effect. (right) Additional features that appear in the pulse height spectrum from the end effect. See the text for an
explanation of the consequences.

pulse height spectrum between the limiting minimum energy and the full energy peak. The wall effect forms
a “valley” between the radiation background (and electronic noise) and the neutron reaction pulse height
spectrum and is a natural location to set the lower level discriminator (LLD).

End Effect The wall effect appears in a spectrum regardless of the geometry for a 3 He detector if any portion
of it is placed in a neutron field. However, if the detector is entirely immersed in a neutron field, another
effect, which is often called the end effect, can also be observed. Many gas-filled proportional counters have
long insulating stand-offs or field tubes at the ends designed to reduce leakage current, arcing, and spurious
counts (see Fig. 17.5). These structures reduce the electric field below the critical field strength necessary
for impact avalanche ionization. Hence, these low field regions operate more like an ion chamber instead
of a proportional counter. Ionization produced in the low field region appears in the lower energy spectral
channels and usually does not contribute to the output signal.
Included in Fig. 17.6 are additional reaction product trajectories that produce the end effect. Trajectories
H and I are cases in which a neutron reaction occurs in the high field region near the low field region, in
Sec. 17.3. Gas-Filled Slow Neutron Detectors 825

which one particle deposits some energy in the low field region and the other particle deposits all energy in
the high field region. Hence, the low field region forms a virtual wall effect, essentially having the same effect
as cases D and E. Similarly, the trajectories of F and G have the
same effect as cases B and C. Additional effects, however, are 0.764 MeV
background
from trajectories J and K, along which a neutron is absorbed in

Counts per Channel


the low field region and only one particle emerges into the high
field region. The case is analogous to the self-attenuation effect 0.573 MeV
observed with neutron reactive coatings. Variations of cases J
and K produce a continuum of energies in the pulse height spec- 0.191 MeV
end effect
trum ranging from zero up to each of the reaction product ener- counts
gies (either 0.191 MeV or 0.573 MeV), thereby forming a reverse
stair step spectrum from that of the wall effect (see Fig. 17.6).
Finally events described by trajectory L are essentially lost. The
added counts appear in the pulse height spectrum in the low en-
ergy valley (or gap) region between the background counts and
Channel Number (energy)
the wall effect spectrum. Further, the end effect adds pulses to
the lower portion of the wall effect spectrum, consequently en- Figure 17.7. Depiction of the main features ex-
hancing that part of the spectrum. The main spectral features pected in a pulse height energy spectrum from a
3
expected from a combination of the wall and end effects are de- He gas-filled neutron detector. End effect counts
are depicted in light gray.
picted in Fig. 17.7.
The end effect is less likely to appear in detector configurations in which a beam of neutrons is incident
perpendicularly to the cylindrical side of the detector. However, for detectors operated in a radiation field in
which neutrons interact more or less uniformly over the detector volume, the end effect is likely be observed.
Shown in Fig. 17.8 are two spectra for different irradiation conditions. The gray spectrum is the result of a
collimated thermal-neutron beam intersecting perpendicular to the central region of the detector of Fig. 17.5.
In this spectrum, features of the main wall effect are discernible, but end effect features are absent. The
white spectrum of Fig. 17.8 is a summed composite in which the collimated thermal-neutron beam was
stepped along the detector length at 5 mm intervals from the end to end, which shows the combined spectral
features from both the end and wall effects.
Both the wall effect and end effect features increase with surface to volume ratio of a detector. Hence,
both of these effects become less prominent for large volume 3 He detectors. However, the spectral energy
resolution of larger detectors is usually lower than smaller counterparts.

10
BF3 Gas-Filled Detectors
Another gas of interest for neutron detection is BF3 , introduced in 1939 [Korff 1939; Korff and Danforth
1939; see review by Wilpert 2012]. Neutrons interact with the 10 B and cause the spontaneous ejection of the
reaction products of Eq. (17.18). These reaction products ionize the host gas, 10 BF3 , in the same manner
as reaction products emitted in a 3 He detector. To increase interaction efficiency, modern BF3 detectors
usually have an enrichment of about 96% in 10 BF3 .
Much like 3 He gas-filled detectors, 10 BF3 gas-filled proportional counters also show wall and end effects
in the pulse height spectra. Because there are two reaction product branches, there is the possibility of
observing four wall effects features, as shown in Fig. 17.9. However, the energy resolution of a 10 BF3 usually
is not adequate to clearly define the 6% branching ratio wall effect features at 1.05 MeV and 1.78 MeV (see
Fig. 17.10). The resulting pulse height spectrum is formed from the reaction products and is not defined
by the energy of the absorbed neutrons. However, good spectral energy resolution assists with defining
an appropriate location for the LLD, thereby allowing pulse height discrimination between neutron and
826 Slow Neutron Detectors Chapt. 17

Figure 17.8. Comparison of pulse height spectra from a 3 He gas-filled neutron detector
irradiated with a thermal-neutron beam directed perpendicular through the center (gray)
and a composite spectrum from neutron irradiations at incremental positions along the
length (white). The detector was a 2 inch diameter, 6 inch long 3 He detector pressurized
to 4 atm, which had insulating standoffs >2 cm long at each end. Both wall and end
effects are apparent in the composite spectrum.

gamma-ray events. For most applications, the LLD is set in the valley between the wall effect features and
the background counts (see Fig. 17.9).
The pressure of the BF3 gas affects the observed energy resolution of the detector, and ultimately
works to limit the maximum neutron detection
efficiency. A study by Fowler [1963] clearly
2.31 MeV
showed spectral deterioration as BF3 gas pres-
sure was increased from 0.131 atm (or 13.33
background
kPa) up to 0.789 atm (80 kPa), in which the
Counts per Channel

94% full energy peak FWHM broadened from


8% up to 56%. Although the detector contin- 1.78 MeV
1.47 MeV
ued to register counts at the higher pressures, 0.84 MeV
1.05 MeV
the energy resolution was poor, which under
end effect
some circumstances remains important for neu- counts
tron detection. Described by Fowler [1963], the 2.79 MeV
best performance was observed for backfill pres-
sures near 0.26 atm (26 kPA). Unfortunately,
Channel Number (energy)
at these low pressures, the advantage of using
10
the high absorption of BF3 gas is compro- Figure 17.9. Depiction of the main features expected in a pulse
mised, yielding typically lower efficiencies than height spectrum from a 10 BF3 gas-filled neutron detector. End effect
observed with common 3 He gas-filled detectors. counts are depicted in light gray.
Sec. 17.3. Gas-Filled Slow Neutron Detectors 827

The efficiency of a BF3 gas-filled detector can be estimated by calculating the total neutron absorption
in the 10 B gas region within the active volume of the detector [Sampson and Vincent 1971],
 10 
)M B
−xi Σit (E) Σa (E)
(E) = e (1 − e−LΣt (E) ), (17.26)
i=1
Σ t (E)

where Σit (E) and xi denote the macroscopic total cross sections and thicknesses of the ith (i = 1 . . . M )
non-sensitive regions, L is the length of the sensitive BF3 gas volume, and where
10 10 11
B B B
Σ t = Σa + Σs + Σt + ΣF Ar
t + Σt (17.27)

with t, s, and a denoting the total, scattering, and absorption cross sections of the homogeneous gas compo-
nents. Note in the approximation of Eq. (17.26), all scattered neutrons are neglected and are assumed not
to produce any subsequent counts.
BF3 detectors can be acquired with relatively thin entrance windows at one end, which allows the long
axis of the detector to be pointed towards the neutron source. Such devices have increased absorption in the
sensitive volume and improved detection efficiency. However, many BF3 detectors are designed with thick
end caps, along with relatively large insulating standoffs for the central wire, thereby producing significant
dead regions at the ends. Consequently, pointing such a device towards the neutron source may reduce
the count rate and observed detection efficiency. Hence, when modeling a detector for a particular neutron
detection application, one must be aware of the orientation of the detector with respect to the neutron source.
Most commercial manufacturers do not quote efficiency for BF3 gas-filled detectors in percent efficiency, but
rather as cps/nv (counts per second per unit thermal-neutron flux), and are evaluated with the entire detector
irradiated with neutrons incident from all directions, a condition in which Eq. (17.26) is inaccurate and not
applicable.

Example 17.1: Consider a 2200-m/s neutron beam of 10-mm diameter intersecting a 10 BF3 gas-filled
detector with the following specifications: 25-mm inner diameter, 2 mm thick Al cylindrical casing, 0.8 atm
pressure, 250 mm total length with anode wire insulating standoffs each 20 mm long at the ends. Assume an
enrichment of 96% 10 B with a fill pressure of 0.8 atm. The density of BF3 is 2.76 mg cm−3 at 1 atm and the
molar mass is 67.82 g mol−1 . What is the thermal-neutron intrinsic efficiency if the neutron beam intersects
perpendicular to the BF3 detector midsection? Afterwards, if the detector is pointed endwise directly at the
neutron beam, what is the thermal-neutron intrinsic detection efficiency?

Solution:
10
First, determine the macroscopic absorption cross section for the B atoms,
10
B 0.96P σρNa 0.96(0.8 atm)(3844 b)(0.00276 g cm−3 )(6.022 × 1023 mol−1 )
Σa = =
A 67.82 g mol−1
= (1.88 × 1019 10
B cm−3 )(3844 × 10−24 cm2 ) = 0.0723 cm−1

The total 2200-m/s cross section of Al is 1.68 b so the macroscopic absorption cross section of Al is,

σρNa (1.68 × 10−24 cm2 )(2.7 g cm−3 )(6.022 × 1023 mol−1 )


ΣAl
t = = = 0.101 cm−1 .
A 26.98 g mol−1
10
Here it is assumed that attenuation from F and 11 B in the gas is negligible, i.e., Σt ≈ Σa B , and all neutrons
absorbed by the 10 B in the gas produce a detectable count. Because the beam diameter is small, the incident
828 Slow Neutron Detectors Chapt. 17

neutrons all pass through 0.2 cm of Al to enter the tube. Then from Eq. (17.26)
Al 10 B
cm)(0.101 cm−1 ) cm)(0.0723 cm−1 )
 = [e−xΣt ][1 − e−DΣa ] = [e−(0.2 ][1 − e−(2.5 ] = 0.162.

Hence, the maximum intrinsic detection efficiency is 16.2% for a crosswise thermal-neutron beam. Absorption
or scattering with the detector tube and F in the gas, along with unfavorable reaction product trajectories,
causes the efficiency to be lower than this ideal case.
Turning the detector lengthwise into the beam, the neutron sensitive region is only 210 mm long with
20 mm dead regions at each end,
Al 10 B 10 B
 = [e−xAl Σt ][e−x10 B Σa ][1 − e−LΣa ]

cm)(0.101 cm−1 ) cm) (0.0723 cm−1 ) cm)(0.0723 cm−1 )


= [e−(0.2 ][e−(2 ][1 − e−(21 ] = 0.662.

yielding 66.2% intrinsic thermal-neutron detection efficiency.

Although 10 B is a 1/v neutron absorber with a relatively high thermal neutron absorption cross, the
absorption efficiency for epithermal neutrons is quite low. The efficiency for these higher energy neutrons
can be increased by increasing the gas pressure, but pressurizing the gas above about 1 atm unfortunately
compromises detector performance and energy resolution; hence, it is usually avoided. Consequently, most
BF3 detectors are limited mainly to slow neutron detection.
Argon gas is sometimes added to BF3 gas-filled detectors, mainly because the Ar (a common proportional
gas) helps preserve the spectral energy resolution [Fowler, 1963; Padalakshmi and Shaikh 2008]. Most com-
mercial detectors have significantly more Ar gas in the detector tube than actual 10 BF3 gas and have pressure
ratios greater than about 40:1 Ar:BF3 . The addition of Ar reduces the avalanche voltage, decreases the gas
multiplication and shifts the counting plateau to lower voltages. For instance, as detailed by Padalakshmi
and Shaikh [2008], the addition of 100 torr Ar to a vessel filled with 10 torr BF3 effectively reduced the
average ionization energy from 35.5 eV for pure BF3 gas down to 26.8 eV for the mixtures of BF3 and Ar
mixture. Hence, equivalent avalanche gains appear at much lower operating voltages for the BF3 and Ar
mixture at 110 torr than for the pure BF3 gas at 10 torr, despite the total gas pressure being increased by
more than a factor of 10. Further, the onset of the high voltage counting plateau was observed to decrease
for the BF3 and Ar mixtures below that observed for the pure BF3 gas samples. Padalakshmi and Shaikh
[2008] note that excellent resolution and stable operating performance was observed for mixtures between
600–800 torr Ar and 100 torr BF3 . Fowler [1963] notes that the increased pressure of a BF3 and Ar mixture
suppresses the wall effect while retaining good energy resolution.
An increase in the pressure of the BF3 within the gas chambers increases the probability of neutron
absorption (and detection efficiency), but also causes the maximum gain of the detector to decrease as a
function of voltage. For instance, Fowler [1963] reports an avalanche gain of 100 achieved with 1000 volts bias
for 10 torr BF3 , but to achieve the same gain at 600 torr BF3 required a bias of 6000 volts. Further, electron
attachment and columnar recombination become problematic at higher pressures and ultimately cause the
formation of smaller electronic signals. Although BF3 and Ar mixtures can be adjusted to achieve optimal
results at a given total pressure, the general trend indicates that at a set applied voltage the avalanche gain
decreases with BF3 partial pressures above 10 torr, and increasing the BF3 pressure also causes degradation
in spectral energy resolution. Typical pressures average about 600 torr for commercial BF3 detectors, but
detectors can be acquired with pressures ranging from 100 torr up through 1300 torr.
As with most proportional counters, BF3 detectors have dead times on the order of tens of mi-
croseconds, which ultimately limits the practical pulse mode count rate to less than about 2 × 104
Sec. 17.3. Gas-Filled Slow Neutron Detectors 829

cps before dead time issues be-


come troublesome. At low
count rates with low probabil-
ity of pulse pile-up, the spectral
features remain recognizable.
However, as the count rate in-
creases, the spectral features
become smeared because of
multiple coincident events dis-
torting the pulse height spec-
trum, as shown in Fig. 17.10.
Another feature of BF3 detec-
tors is that the gas becomes ex-
hausted over an extended oper-
ation time. Qian et al. [1998]
report performance degrada-
tion due to gas depletion ap-
pearing for total neutron inter-
Figure 17.10. Pulse height spectrum from a 10 BF3 gas-filled neutron detector at low actions in the detector gas be-
(shaded region) and high (dotted line) neutron interaction rates. The detector was
irradiated with a collimated thermal-neutron beam intersecting the mid-section; hence,
tween 1010 and 1011 . Depend-
end effects are not apparent. The wall effect features at 1.05 MeV and 1.78 MeV are not ing on the size of a BF3 detec-
easily discernible. tor, typical operating voltages
may range from 500 volts for
small diameter detectors (about 12 mm) up to 3000 volts for some large diameter detectors (about 50 mm).
Also, usually quoted operating temperatures range from -50 ◦ C to 100 ◦ C. Operating the detectors at much
higher temperatures than room temperature degrades energy resolution, and in some cases, at elevated
temperatures, appears to cause irreversible damage.
BF3 gas is designated as a level 3 health hazard by the National Fire Protection Association (NFPA
704). This classification means that short exposure to the gas can cause serious temporary or residual
injury. Many organizations have abandoned the use of 10 BF3 primarily because of the health risks. Because
of the toxic nature of BF3 gas, the government has imposed special restrictions on the transport of these
devices; however, because 10 BF3 detectors are an important type of neutron detector, there is not a complete
ban on the shipping of certain types of these detectors. The International Air Transport Association (IATA)
Special Provision A190 permits the aircraft shipment of BF3 detectors containing more than 1 gram up to
12.8 grams of BF3 and filled to pressures no more than 105 kPa absolute at 20◦ C. It also applies to radiation
detection systems containing up to 51.2 grams of BF3 . The U.S. Department of Transportation (DOT)
special provision 238 basically reiterates the same provisions. Overall, these detectors must be packed in a
sealed plastic bag or plastic liner along with an absorbent capable of absorbing all of the gas contained in
the detectors should the gas detector leak during transportation. Detector manufacturers can obtain special
transport permits for detectors with higher BF3 mass and gas pressures than allowed by IATA SP A190 or
DOT SP 238.10

17.3.2 Detectors with Neutron Reactive Coatings and Layers


The class of neutron detectors that incorporate reactive materials as coatings on the walls, or reactive inserts
inside the gas container, are often called coated neutron detectors. This term actually applies to variations

10 IATA SP A190 and DOT SP 238 were still effective at the time of writing this book.
830 Slow Neutron Detectors Chapt. 17

Figure 17.11. (left) The Bragg ionization curve for pure 10 B material, showing the specific ionization of 10 B(n,α)7 Li
reaction products as they pass through the material. (right) The residual energy retained by 10 B(n,α)7 Li reaction products
as they pass through pure 10 B material [from McGregor et al. 2003].

of coated gas-filled, scintillator, and semiconductor neutron detectors, and the basic analysis applies to all,
with minor differences.
It is important to note that the charged particles have discrete ranges within a material, and they lose
energy as a function of the specific stopping power of the material through which they pass. Charged
particle energy loss is not linear with distance, and the energy loss for high-energy heavy charged particles
can generally be described by Eq. (4.147). For non-relativistic particles this equation reduces to
 
1 dE 4πz 2 e4 me v 2
− = Z ln , (17.28)
N dx 4π2o me v 2 I
in which ze is the charge of the heavy ion, v(x) the speed of the charged particle after traveling a distance
x, N is the atomic density, me is the rest mass of an electron, Z is the material atomic density, and I
is an experimentally determined mean excitation energy describing the average excitation potential of a
representative atom in the material.
Although the average range is treated as constant, the actual range fluctuates from particle to particle
because of deviations in the number of Coulombic scatters per unit distance and deviations in energy loss
per collision. The fluctuation may exceed 5% of the total range, and this fluctuation is referred to as the
straggle in the particle range. Recall from Fig. 4.26, Rp is the mean
√ or average range and Re > Rp is the
extrapolated range. The slope of the fraction reaching Rp is 1/(α π) so that the two ranges are related by

π
Rp = Re − α. (17.29)
2
A Bragg curve is a plot of the ionization versus penetration distance, averaged over a large number of
individual identical source ions. Let I(x) be the Bragg curve ordinate, i.e., the average ionization per unit
differential path length at a distance x from the source. Then I(x), accounting for straggling, is [Evans 1955]
 ∞
i(r − x)
I(x) = √ exp[(Rp − r)/α]2 dr, (17.30)
x α π
where i(r − x) is the specific ionization (LET) along the path of an individual particle at a distance (r − x)
from the end of its path, and x is the distance an individual particle is from the source. An interesting
Sec. 17.3. Gas-Filled Slow Neutron Detectors 831

Figure 17.12. (left) The Bragg ionization curve for pure 6 Li metal, showing the specific ionization of 6 Li(n,t)4 He reaction
products as they pass through the metal. (right) The residual energy retained by 6 Li(n,t)4 He reaction products as they
pass through pure 6 Li metal [from McGregor et al. 2003].

Figure 17.13. (left) The Bragg ionization curve for pure 6 LiF material, showing the specific ionization of 6 Li(n,t)4 He
reaction products as they pass through the material. (right) The residual energy retained by 6 Li(n,t)4 He reaction products
as they pass through pure 6 LiF material [from McGregor et al. 2003].

characteristic of the Bragg ionization curve for alpha (α) particles is the increase in columnar ionization per
unit volume as the ion energy decreases. Hence, the highest density of electron-hole pairs is excited near the
end of the range for α-particles.
In the present treatment the average effective range, denoted by L, is the distance through which an ion
may travel within the neutron reactive film before its energy decreases below the set minimum detectable
threshold, typically defined by the electronic lower-level-discriminator (LLD) setting. The effective range L
does not take into account additional energy losses from contact “dead regions”. LSR and LLR denote the
average effective ranges for the short-range and long-range reaction products, respectively. The graphs of
Fig. 17.11, Fig. 17.12, and Fig. 17.13 can be used to determine the reaction product effective ranges as a
function of LLD for pure enriched 10 B, 6 Li, and 6 LiF, respectively.
832 Slow Neutron Detectors Chapt. 17

Neutrons may interact anywhere within the reactive film. From Fig. 17.11, Fig. 17.12, and Fig. 17.13, it
is apparent that the reaction products also lose energy as they move through the reactive film, thus limiting
the energy that can be transferred to the detector gas (or semiconductor material). The finite specific energy
loss in the reactive film limits the usable film thickness that can be deposited on the walls of the gas chamber
or over the semiconductor device. The voltage signal measured is directly proportional to the number of ion
pairs created within the detector gas or semiconductor. Reaction products that deposit most or all of their
energy in the active volume (the gas or semiconductor where ionization is recorded) produce much larger
voltage signals than those reaction products that lose most of their energy in the surface films and contacts.
The neutron flux transported through the film a
DF
distance x, ignoring neutron scattering, is
neutron I(x) = Io exp[−xσa Na ] = I0 exp[−xΣa ]. (17.31)
reactive film

where I0 is the initial neutron flux, Na is the


atomic density of the neutron reactive isotope in
the film, σa is the microscopic thermal-neutron
absorption cross-section of the film, and Σa is
neutron L
the film macroscopic thermal-neutron absorption
x cross section. The fraction of neutrons absorbed
detector in the film while traveling a distance dx about x
volume
neutron is,
interaction
location p(x)dx = Σa exp[−xΣa ]dx. (17.32)
Besides the attenuation of neutrons as they travel
in the reactive film, the reaction products are also
attenuated as they traverse the reactive film. This
particle entrance
ion self-attenuation depends on the ion emission
solid angle angle with respect to the normal of the film. Once
Figure 17.14. The solid angle formed by a reaction product range
a neutron is absorbed and the reaction products
that subtends the detector at the interface determines the neutron are emitted, the probability that a reaction prod-
detection probability. uct enters the detector is determined by the solid
angle subtending the surface within the average
effective range L of the reaction particle. From Fig. 17.14, a neutron interaction taking place at distance x
from the semiconductor surface has a probability of entering the active volume equal to the fractional solid
angle that subtends the detector, i.e.,
   
Ω(x) 2π x x
pp (x) = = 1− = 0.5 1 − , x ≤ L, (17.33)
4π 4π L L
where the subscript “p” refers to the reaction ion of interest. Because the reactions of interest in the present
work release two different reaction products per event, the total probability of detecting a neutron reaction
consists of adding the detection probabilities of both reaction products. Note that at some interaction
locations only one reaction product may be able to reach the active volume of the detector.
Efficiency Analysis for Detectors with 10 B, 6 Li, or 6 LiF Coatings
First consider a simple case. Suppose a layer of neutron reactive material is placed within gas-filled detector
upon an inside surface, as depicted in Fig. 17.15. The thermal-neutron reactive materials 10 B and 6 Li emit
these reaction products in opposite directions; hence, only one of the particles can enter the detector gas.
The neutrons may be absorbed in the neutron reactive coating on the entry side of the detector (cases A, C,
Sec. 17.3. Gas-Filled Slow Neutron Detectors 833

detector neutron neutron detector


wall reactive reactive wall
coating coating
entry exit
surface either reaction surface
product can
enter the gas
A
detector
gas
B
only the long
range particle
can enter the gas
C only the long
range particle
neutron
can enter the gas

E neither particle
either reaction
can enter the gas
product can
enter the gas

x x
D 0 0 D
Figure 17.15. Escape of reaction products from a neutron reactive film coating inside the gas-filled region
of a detector.

and E in Fig. 17.15), or may pass through and become absorbed in the neutron reactive coating on the exit
side of the detector (cases B and D in Fig. 17.15), or may pass through the detector without being absorbed.
Consider cases in which neutrons interact with the coating on the entrance side in the gas-filled detector.
Because the reaction products are emitted in opposite directions for thermal neutron absorptions, only one
reaction product per event can enter the detector active region. Each reaction product can be analyzed
separately and the results are subsequently summed to determine the total detection efficiency. Situation
A in Fig. 17.15 depicts the case in which either reaction product can enter the gas region of the detector,
and situation C depicts the case in which only the long range reaction product can reach the detector gas.
Situation E depicts that case in which neither reaction product can reach the active volume of the detector.
Note that the calculation must account for any neutron interactions in the detector wall, because those
neutrons are lost before entering the detector and, consequently, reduce the overall detection efficiency.11
For the coordinate orientation for the entry surface shown in Fig. 17.15, Eq. (17.32) and Eq. (17.33) are
multiplied and integrated over the coating thickness D to find the efficiency for each reaction product. Here
the neutrons are assumed to be normally incident on the wall. Also the wall/coating interface is placed at

11 Actually,
some wall scattered neutrons do reach the detector gas and may produce a count. Thus, the analysis in this section,
which treats a scatter as an absorption, represents a lower bound on the detector efficiency.
834 Slow Neutron Detectors Chapt. 17

x = 0 so that y = D − x. If the overall coating thickness D is less than the reaction product effective range
L, the sensitivity contribution (or probability of entering the detector gas or semiconductor) of that reaction
product is,
  
Fp ) −Σit Ti D
M
−Σa (D−x) x
SP (D) = e 2πΣa e 1− dx,
4π i=1 0 L
)M  
−Σit Ti 1 D
= 0.5Fp e 1+ (1 − e−Σa D ) − , D ≤ L, (17.34)
i=1
Σa L L
where Fp is the branching ratio of the reaction product, Σit and Ti denote the different material total
thermal macroscopic cross sections and thicknesses of those materials through which neutrons must pass
before encountering the reactive coating, M is the number of these materials encountered, D is the thickness
of the reactive coating, Σa is the macroscopic thermal-neutron absorption cross section of the reactive coating,
and L is the effective range of the reaction product.
If the overall coating thickness D is greater than the reaction product effective range L, the self-absorption
neutron losses within the entry coating layer must be included. The sensitivity contribution of that reaction
product is, for D > L,
  
Fp e−Σa (D−L) ) −Σit Ti L
M
x
SP (D) = e 2πΣa e−Σa (D−x) 1 − dx
4π i=1 0 L
)M  
−Σa (D−L) −Σit Ti 1
= 0.5Fp e e 1+ (1 − e−Σa L ) − 1 . (17.35)
i=1
Σ a L
For a cylindrical tube detector, neutrons that do not interact in the coating as they enter the detector
may transit the detector gas and interact in the coating on the opposite surface, as shown by cases B and D
in Fig. 17.15. These interactions with neutrons interacting with the exit surface of the detector can produce
additional detectable events that must be added to the events recorded for interactions with the coating on
the entry surface. The analysis is simplified if the axis is reversed, as shown in Fig. 17.15 for the exit surface.
Eq. (17.32) and Eq. (17.33) are multiplied and integrated over the coating thickness D to find the efficiency
for each reaction product. If the coating thickness D is less than the reaction product effective range L, the
sensitivity contribution of that reaction product is, for D ≤ L,
  
Fp e−Σa D ) −Σit Ti D
M
x
SP (D) = e 2πΣa e−xΣa 1 − dx,
4π i=1 0 L
)M  
−Σa D −Σit Ti 1 D
= 0.5Fp e e 1− (1 − e−Σa D ) + e−Σa D , (17.36)
i=1
Σa L L
where losses in the entrance coating are included. If the coating thickness D is greater than the reaction
product effective range L, the sensitivity contribution of that reaction product (also accounting for reaction
product losses in the entrance surface coating) is
  
Fp e−Σa D ) −Σit Ti L
M
x
SP (D) = e 2πΣa e−xΣa 1 − dx,
4π i=1 0 L
)M  
1
= 0.5Fp e−Σa D e−Σt Ti (1 − e−Σa L ) + e−Σa L .
i
1− (17.37)
i=1
Σ a L
Sec. 17.3. Gas-Filled Slow Neutron Detectors 835

Usually a coated gas-filled detector is backfilled with a gas that is relatively unreactive with neutrons;
hence it is usually neglected in sensitivity calculations. However, if the gas is an absorber of neutrons,
then those losses imposed by the gas must also be taken in account. After the sensitivity components are
calculated for all reaction products and branching ratios, they are summed to determine the intrinsic neutron
detection efficiency, i.e.,
   
M
 M

int = Sp (D) + Sp (D) . (17.38)
p=1 entry p=1 exit

Example 17.2: Consider a two-inch inner diameter gas-filled detector backfilled at 1 atm with P-10
counting gas. The detector is fabricated from 2-mm-thick Al tube. The walls are coated with D = 10
microns of γ = 94% enriched 6 LiF. The detector is best operated with the LLD set to an equivalent of 250
keV. For a 1-cm diameter beam of 2200 m s−1 neutrons intersecting perpendicularly through a cross section
of the detector, what is the expected neutron detection efficiency int ?

Solution:
The mass density of common LiF is 2.635 g cm−3 and the atomic weight is A = 25.939. From these data
the macroscopic cross section of the 6 LiF material is found as
σa γρNa
Σa = σa N =
A
(938 × 10−24 cm2 )(0.94)(2.635 g cm−3 )(6.022 × 1023 mol−1 )
= = 53.9 cm−1 .
25.939 g mol−1

The residual energy graph (at an LLD of 250 keV) for pure enriched 6 Li, shown in Fig. 17.13, is used
here to estimate the values of L, with Lα ≈ 4.8 microns and Lt ≈ 29.5 microns even though the density
used in the figure is slightly different than in this problem. Because Lt > D, Eqs. (17.34) and (17.36) are
used to determine the triton contribution to the efficiency. The 2200-m/s total microscopic cross sections
for Al and Ar are 1.68 b and 1.32 b, respectively; hence, it is assumed that 2 mm of Al and 5 cm of Ar at 1
atm have little effect on neutron losses and can be neglected. Further, the branching ratio for the reaction
products is 100%; hence, Fp = 1. Equations (17.34) and (17.36) reduce to
  

 1 D
SP (D) = 0.5 1 + (1 − e−Σa D ) − ,
 Σa Lt Lt
entry
 
1 −1 −3
= 0.5 1 + 1 − e−(53.9 cm )(10 cm)
(53.9 cm−1 )(29.5 × 10−4 cm)
10−3 cm
− = 0.0218.
29.5 × 10−4 cm
  

and  1 D −Σa D
SP (D) = 0.5e−Σa D 1− (1 − e−Σa D ) + e = 0.0207.
 Σa Lt Lt
exit

Because Lα < D, Eqs. (17.35) and (17.37) are used to determine the alpha particle contribution to efficiency,
which along with the previous assumptions, yield
  

 −Σa (D−Lα ) 1
SP (D) = 0.5e 1+ (1 − e−Σa Lα ) − 1 = 0.0062,
 Σa Lα
entry
  
and 
 1
SP (D) = 0.5e−Σa D 1− (1 − e−Σa Lα ) + e−Σa Lα = 0.0061.
 Σa Lα
exit
836 Slow Neutron Detectors Chapt. 17

These results are summed to determine


 the intrinsic
 efficiency,
M  M 
 
int = Sp (D) + Sp (D) = 0.0218 + 0.0062 + 0.0207 + 0.0061
p=1
 p=1

entry exit
= 0.0548 or 5.5%.

Self-Attenuation Effect
Because the reaction products are released in opposite directions, only one of these particles can enter the
gas region, as explained previously. Consequently, the pulse height spectrum extends from zero up to the
highest energy of any single reaction product. The fact that energy can be lost by a reaction ion before
depositing the remainder of its energy in the gas is known as the “self-attenuation effect”.
Consider the case of a gas-filled detector
thin
wall
coating
with a 10 B coating on the inner cathode sur-
events events face, as depicted in Fig. 17.16. Neutron ab-
Counts

A for B for A
sorptions that occur at the gas/coating inter-
B
face, depicted as cases A and B, allow either
C continua the alpha particle or 7 Li ion to deposit all their
for C
gas
events
energy in the gas. Note that in either case
D continua none of the energy from the other reaction
for B’
for D events
for A’ product is absorbed in the gas, but instead
E Energy is completely lost in the coating and detector
(MeV)
wall. Under no circumstance is the full Q-
0.84 1.05 1.47 1.78 value of the reaction recorded for this detector
lithium ion alpha particle
wall thick events
configuration. For all interactions that occur
continua
coating
A for D for B events deeper in the 10 B coating, depicted by cases
Counts

for A
C and D, energy self-attenuation lowers the
events
B for B’ amount of energy registered for those parti-
continua
for C cles that emerge into the detector gas. Conse-
C quently, these events appear at lower energies
gas in the pulse height spectrum and range from
events
D for A’ zero up to the full energy of the four possi-
Energy
ble reaction product energies. Case E depicts
E
(MeV) those events in which neither particle emerges
0.84 1.05 1.47 1.78 into the detector gas; hence the events are not
recorded.
Figure 17.16. Escape of reaction products and spectral features
for a gas-filled detectors with thin (upper) and thick (lower) 10 B
For thin 10 B coatings, the probability of
coatings. The 94% branching ratio energies are represented by A case E occurring is relatively low, and energy
and B, and the 6% branching ratio energies are represented by A self-attenuation is minimized, thereby allow-
and B . ing spectral features of the energies of the dif-
ferent reaction products to appear in the pulse height spectrum, as depicted in Fig. 17.16. For thick 10 B
coatings, these spectral features are lost, and instead a “stair-step” spectrum is produced. The stair-step
feature is a consequence of the combined effects of solid angle, interaction depth, and energy self-attenuation.
The resulting probability of depositing energy between zero and the maximum is approximately constant for
each reaction product, thereby producing a rectangular shaped pulse height spectrum for each reaction prod-
uct, that when added together forms the familiar stair-step spectrum. The calculated results for different
converter thicknesses of a 10 B-lined detector are shown in Fig. 17.17.
Sec. 17.3. Gas-Filled Slow Neutron Detectors 837

10
B-Lined Tubes
Detectors coated with 10 B, generally called boron-lined detectors, and (along with lithium-lined detec-
tors) are perhaps the first type of gas-filled slow neutron detectors introduced to the scientific com-
munity [Dunning et al. 1935a; Mitchell 1936].12 They are commercially available with casings usu-
ally constructed from either aluminum or stainless steel. The coatings, in units of mass thickness,
range from 0.025 mg cm−2 up to 1 mg cm−2 or in thicknesses of 0.1 micron up to 4.33 microns.
Coatings thicker than 4.6 microns are greater than the range of the most penetrating reaction prod-
uct (see Fig. 17.11) and do not increase the detection efficiency but serve only to reduce the neutron
flux. The thicker coatings, often quoted with mass thicknesses between 0.5 and 1.0 mg cm−2 , pro-
duce pulse height spectra with the self-attenuation stair-step feature shown in Figs. 17.16 and 17.17.
Efficiency is usually quoted in units of total
count rate from the detector per unit flux
(cps/nv), with the detector completely im-
mersed in a neutron field. If used in a neutron
beam, the orientations described in Example
17.1 and method of Example 17.2 should be
used to estimate the expected efficiency.
Boron-lined tubes are available in various
sizes, with diameters usually ranging from 13
mm up to 77 mm. Because neutrons interact
in the coating attached to the walls, detectors
are designed for irradiation through the side
wall; hence, there is dead space near the tube
ends from the insulating standoffs and/or field
tubes.
Boron-lined gas-filled detectors can use
practically any counting gas, an advantage Figure 17.17. Pulse height spectra for a boron-lined detector for
over detectors based on 3 He or 10 BF3 gases. three boron layer thicknesses. Although the total number of reg-
Boron-lined tubes designed as ion chambers istered counts increases with boron thickness, the self-attenuation
can be commercially acquired with hydrogen effect is also enhanced and degrades the reaction product spectrum.
as the backfill gas, while boron-lined proportional counters are usually backfilled with traditional propor-
tional gases such as argon. Boron-lined gas-filled detectors compensated for gamma-ray background can be
acquired with a variety of fill gases, including hydrogen, nitrogen, and xenon. Boron-lined tubes can be used
under relatively higher temperature conditions (up to about 200◦C) than is possible with 10 BF3 gas-filled
detectors.
Unfortunately, the self-attenuation effect limits boron-lined gas-filled neutron detectors to approximately
9% maximum intrinsic thermal-neutron detection efficiency, much lower than that measured for 3 He or 10 BF3
gas-filled detectors. Neutron measurements often require the LLD be set to reduce gamma-ray background
counts. Unfortunately, any non-zero setting of the LLD also eliminates neutron counts, effectively reducing
the detection efficiency below the maximum possible. This problem is a consequence of the reaction product
self-attenuation, which produces no “valley” feature in the pulse height spectrum in the low energy region
(unlike 3 He or 10 BF3 gas-filled detectors). Detectors with axially aligned 10 B-coated fins, inserts, or hon-
eycomb structures inside a boron-lined tube have been investigated as a method to increase the efficiency
[McGregor et al. 2013a; Nelson et al. 2012, 2014; Edwards et al. 2018]. The total neutron detector efficiency
increases with the added boron-coated surface area in the gas chamber.

12 Curie and Joilet [1933] and Bonner [1933] had already shown that ionization by neutron recoil collisions can be detected.
838 Slow Neutron Detectors Chapt. 17

Compensated Ion Chambers


A form of ion chamber widely used for nuclear reactor controls is the compensated ion chamber. Ion chambers,
when operated in current mode, can be used in high radiation environments. If a gas-filled neutron detector
is placed near a nuclear reactor, it responds to both neutrons and gamma rays. Yet, current mode operation
does not permit pulse height discrimination between neutron and gamma-ray interactions as does pulse mode
operation. The compensated ion chamber design is used to distinguish between the two types of radiations.
Typically the chamber has three concentric elec-
g-ray sensitive trodes, one coated with a neutron sensitive material
chamber volume Ig - + such as 235 U or a compound containing 10 B. As seen
from Fig. 17.18, the 10 B (or 235 U) coated chamber is
generally referred to as the “working” chamber and the
central
electrode
uncoated chamber is referred to as the “compensat-
ing” chamber. When exposed to a combined gamma-
ray and neutron source, the voltage potential for the
Ar gas working chamber causes current to flow that deflects
the meter in one direction. The voltage potential in
In = Ig + n - Ig the compensating chamber, sensitive only to gamma
rays, causes current to flow in the opposite direction.
10
B coating The voltage potentials on the chambers can be ad-
justed so that the two gamma-ray induced currents
neutron and g-ray
are equal. As a result, in the compensating chamber
sensitive chamber volume Ig + n + - the two gamma-ray currents cancel each other so the
Figure 17.18. Cross section diagram of concentric com- net signal is solely from the neutron induced current.
pensated ion chamber. The configuration allows both Compensated ion chambers are widely used in nuclear
chambers to experience the same radiation field. Differ-
reactors because of their ability to respond to neutron
ences between the two chambers can be properly calibrated
by adjusting the operating voltages. fields that vary up to ten orders of magnitude, i.e.,
these detectors have a very large “dynamic range”.

10
B4 C-Coated Straw Tubes
Miniaturized version of the boron-lined neutron detector, dubbed “boron straw tubes”, have been introduced
in recent years [Lacy et al. 2009, 2013]. These detectors have similar properties to those of the straw tubes
described in Sec. 10.6.7. Boron straw tubes are fabricated from either Al or Cu metal foil that has been
coated with BC4 , enriched to approximately 96% 10 B [Lacy et al. 2013]. The BC4 material is applied with
physical vapor deposition (PVD) to produce a durable layer that can withstand shock and relatively high
temperatures. Afterwards, the metal foil is rolled and welded to form the envelope. Each straw tube is
designed as a coaxial detector, with a central anode wire and the metal foil envelope acting as the cathode.
These detectors range in diameter from 2 mm to 15 mm, and can be over 1 meter long, depending on the
design.
A single detector has the same efficiency limitations as any other boron-coated gas-filled neutron detector.
However, because of their relatively low production cost, compact size, and durability, large groups of boron
straw tubes are usually bundled together in a larger vessel, thereby increasing the overall neutron detection
efficiency. Recent designs deviate from the conventional cylindrical tube, adapting instead a “star-shaped”
straw tube. The star shape design increases the overall neutron reactive surface while allowing the straws
to pack together in an interlocking manner [Lacy et al. 2013]. Such a configuration increases the amount
of 10 B-coated surfaces encountered by an intersecting neutron beam. Approximately 31 straw tubes, each
nominally 4.43 mm diameter, can be packaging inside a 1.15 in (29.2 mm) diameter Al tube and operated
Sec. 17.3. Gas-Filled Slow Neutron Detectors 839

as a single detector. Lacy et al. [2016] have also adopted the axial fin design [McGregor et al. 2013a] inside
straw tubes to improve thermal neutron detection efficiency.
A disadvantage of such small geometries is that the reaction product ranges are typically much greater
than the straw-tube cross dimensions. Consequently, much of a reaction product energy is lost when it
encounters an opposing surface; hence only a portion of the reaction energy is actually deposited in the
straw tube, thereby producing a smaller output signal. Energy deposition can be increased by increasing the
pressure inside the straw tube. One advantage of the small size is the reduced ionization in the detectors
from background gamma rays so that the background radiation interference is reduced. Charged particles are
naturally shielded from entering the vessel, and electrons excited through gamma-ray and x-ray interactions
inside a straw tube can not physically deposit much energy (low -dE/dx) before encountering a surface.
Hence, the discriminator can be set lower than that of a conventional boron-coated detector and, thereby
allows more neutron-induced counts to be tallied.
The overall efficiency is a function of the BC4 thickness, enrichment, gas pressure, LLD setting, and
the number of surfaces encountered. Shown in Fig. 17.19 are calculated efficiencies, using a combination
of Eqs. (17.34), (17.35), (17.36), and (17.37) for each 10 B surface encountered in a stack, illustrating the
efficiencies that are achievable by stacking multiple boron-coated straw tubes. For optimal conditions at an
LLD setting of 73 keV equivalent with a neutron beam intersecting perpendicular to the vessel, a 29.2 mm
diameter vessel with 31 round straw tubes can achieve an efficiency exceeding 35%, while 31 star shaped
close packed straw tubes can achieve efficiencies exceeding 50% [Lacy et al. 2013]. These numbers vary with
LLD setting. Presently, boron coated straw tubes are being incorporated into field instruments, including
portal monitors, backpack monitors, and vessels having traditional form factors as those of conventional 3 He
detectors [Lacy et al. 2013].

Gas-Filled Detectors with 6 Li Metal


A relatively new technology that shows great promise is a neutron proportional counter loaded with 6 Li
metal foil sheets, made possible by film advancements by the Li battery industry. These 6 Li foil sheets
can either be attached to the container walls or, more effectively, several 6 Li foil inserts can be suspended
inside the detector chamber. A system of analytical equations can be used to determine the theoretical
efficiencies of stacked detector variations [McGregor et al. 2003] or, instead, Monte-Carlo methods can be
used to determine the expected efficiencies [Nelson et al. 2012].
Relatively large neutron detectors can be constructed by laminating the walls of a chamber with thin 6 Li
foils, between each foil a multiwire proportional counter is constructed (see Fig. 17.20). A single detector
box typically has two foils, one on each side, and each additional detector increment adds two more foils.
This type of Li foil detector has similar properties to the boron lined gas-filled detector or any of the coated
detector variants, in which only one of the reaction products from the 6 Li(n,t)4 He reaction can escape into the
detection gas. The efficiency can be calculated using the method introduced by Eqs. (17.34) to (17.37), while
accounting for neutron absorption losses through each detector box. The resulting calculated efficiencies are
shown in Fig. 17.21. Although foils less than 20 micron in thickness can reach thermal-neutron detection
efficiencies exceeding 50%, this value is presently impractical due to limitations with manufacturing the thin
Li foils. Presently, the quoted lower limit is 55 microns,13 and yields a saturated maximum intrinsic thermal
neutron detection efficiency of 47%. Because there are additional neutron losses from the box materials, it
is expected that the actual efficiency is somewhat lower.
Large neutron detectors can also be constructed by suspending framed sheets of 6 Li foils inside a gas-filled
chamber interspersed between multiwire anodes as shown on the right-hand side of Fig. 17.22 [McGregor
et al. 2013a, 2017]. Unlike coated detectors, the thin 6 Li foil may allow both reaction products to reach

13 Source: Rockwood Lithium.


840 Slow Neutron Detectors Chapt. 17

Figure 17.19. Calculated efficiencies for a stack of 10 B-lined tubes irradiated with a thermal-
neutron beam normal to the axis. The efficiency is shown as a function of the 10 B film thickness
and the number of tubes intersected by the thermal-neutron beam.

the detection gas, as depicted in Fig. 17.22. Situation A in Fig. 17.22 depicts the case in which either
reaction ion can enter the gas region of the detector with a small possibility of both ions entering the gas
on opposite sides. Situation B depicts the case in which only the long range reaction product can reach the
detector gas from either side of the foil. Situation C depicts that case in which either one of the reaction
ions can reach the detector gas but not both. The thermal-neutron detection efficiency for this type of
detector can be calculated with the system of equations listed in the literature [McGregor et al. 2003], an
analytical method that can be somewhat tedious. Alternatively, widely used Monte-Carlo codes, such as
MCNP-6 or GEANT-4, can also be used to calculate the thermal-neutron detection efficiency [Nelson et
al. 2012]. The resulting calculated efficiencies are shown in Fig. 17.23. For the minimum 6 Li foil thickness
of 55 microns, a detector with 10 foils can deliver 72% thermal-neutron detection efficiency. The efficiency
reported for 6 Li 5-foil detectors exceeds 56%. It is interesting to note that a 6 Li-foil detector with a single
suspended foil (maximum 24% efficiency) outperforms a two foil detector of the laminated design (maximum
20% efficiency).
The main advantage of the laminated 6 Li design is that each detector box in a stack requires only one
bank of multiwire anodes. However, the laminated design cannot achieve the high efficiency of the suspended
foil design. The main advantage of the suspended foil design is that it can achieve efficiencies similar to those
of 3 He gas-filled detectors. In either case, the detector is backfilled with a proportional counter gas rather
than a rare or caustic reactive gas (which may also not exhibit ideal signal proportionality). A variety of
detector shapes and sizes are described in the literature [Nelson et al. 2012, 2014, 2015].
Although Li foils react and decompose in the presence of water moisture, fabrication problems can be
mitigated by constructing the detectors within a “dry room”, in which water moisture can be kept below
Sec. 17.3. Gas-Filled Slow Neutron Detectors 841

detector detector
Li foil wall wall Li foils anodes
anodes
coatings (cathode) (cathode)

Figure 17.20. For large area Li-foil detectors, there are two basic design constructions. Depicted
are (left) a laminated construction with six 6 Li foils and (right) a suspended construction with
four 6 Li foil inserts in the gas container.

Figure 17.21. Calculated thermal-neutron detection efficiencies for 6 Li foils attached to the
walls of stacked gas-filled chambers.
842 Slow Neutron Detectors Chapt. 17

either reaction
product can
A enter gas - with
small chance of
both products
entering the gas

detector detector
gas gas

B only long range


particle can
neutron enter gas

Li foil

either reaction
C product can
enter gas

Figure 17.22. Escape of reaction products from a thin suspended


foil of 6 Li inside a gas-filled detector.

Figure 17.23. Calculated thermal-neutron detection efficiencies for 6 Li foil


inserts suspended in a gas-filled chamber.
Sec. 17.3. Gas-Filled Slow Neutron Detectors 843

10 ppb. The detectors operate with proportional gases, such as argon. However, it is inadvisable to use
quenching gases that contain oxygen, such as CO2 , because these gases cause the Li foils to decompose over
time. Instead, saturated hydrocarbons such as the linear alkanes methane, ethane, and propane can be
used as quenching gases. To prevent foil decomposition, all gases introduced into the chamber should have
ultra-high purity, generally with less than 1 ppm of either O2 or water moisture contamination.

Fission Chambers
A special type of coated gas-filled radiation detector is a fission chamber. This type of detector has fissile
materials (such as 233 U, 235 U, 239 Pu) or fissionable materials (such as 237 Np, 232 Th, 238 U) as coatings in
which a fission reaction emits two highly energetic fission products. The energy eventually released per
235
U fissioned is approximately 207 MeV, with about 168 MeV of that energy as the kinetic energy of the
two fission fragments. The remaining 39 MeV is released in the form of gamma rays, fast neutrons, beta
particles, and neutrinos, most of which escape detection. Usually two fission fragments share 168 MeV as
kinetic energy, although there is a slight chance of triplet fission, that produces two relatively large fission
products and a much smaller fission product (such as a triton, alpha particle, Li ion, or B ion). The two fission
fragments are released with different kinetic energies and masses, with average energies of 68.1 MeV for the
heavy fragment and 99.2 MeV for the light fragment. The variety of possible fission fragments numbers in
the hundreds with atomic masses ranging from 70 to 170. The fission product mass and energy distributions
for fissile materials (233 U, 235 U, 239 Pu) have similar distributions, although there are slight differences.
Threshold detectors can be used for fast
fission reactions, which include 237 Np,
238
U, and 232 Th to measure only the
fast flux while discriminating epither-
mal and slow neutrons (see Fig. 17.24).
The large kinetic energy of the fis-
sion provides an attractive converter for
neutron detectors, mainly because the
energy from either fission product (frag-
ment) can be measured without the
need for avalanche multiplication. As Th-232
a result, most fission chambers are de-
signed as ion chambers. The ranges of
fission products in 1 atm of Ar are be-
tween 1.5 cm and 2.9 cm, depending
on their mass and energy; hence many
fission chambers are designed with di-
mensions of a few centimeters. In a
fission event, the fission fragments are Figure 17.24. Fast neutron fission cross sections for several materials used for
ejected in approximately opposite di- fission chambers. The isotopes 238 U, 237 Np, and 232 Th are used as threshold
rections, although the other energetic converters, in which neutrons below an energy threshold are unlikely to interact
fission emissions, such as prompt fission in the detector. Data are from [ENDFPLOT 2015]. (The slow neutron cross
sections for 235 U and 239 Pu are shown in Fig. 17.3).
neutrons, cause a slight change in the
opposite fission product trajectories. Consequently, much like other coated neutron detectors, only one of
the fission products is likely to cause ionization of the chamber gas and be measured.
Although the number of electron-ion pairs created in the gas depends on the amount of energy deposited
by the fission fragments, it is also a function of the effective Z of the fission products. The average number
of ion pairs created, per unit energy deposited, is higher for an alpha particle than for fission fragments,
844 Slow Neutron Detectors Chapt. 17

assuming full energy deposition and identical operation conditions [Rao et al. 1990]. This outcome is a
consequence of heavy ions losing energy to competing processes, such as direct nuclear collisions, that do not
produce electron-ion pairs (discussed in Sec. 16.2.7). Hence, the actual pulse height produced by a fission
fragment does not scale linearly with its initial energy, unlike the more linear relation for alpha particles.
Also, the average charge on a fission fragment reduces rapidly as it passes through a medium as the fission
fragment captures ambient electrons. Consequently, the specific ionization of a fission fragment is highest
upon entering a medium and decreases as the fission fragment loses energy. This changing charge of the ion
is quite different than that experienced by alpha particles and protons. Overall, for full energy deposition,
the total amount of energy converted to electron-ion pairs for fission fragments is considerably higher than
observed by alpha particles, beta particles, or gamma rays.
Theoretical models, developed by Kahn et al. [1965], predict the pulse height spectra produced by fission
fragments emitted within a 2π solid angle from a thin film coating of UO2 on a surface within a gas detector.
Selected predictions are compared to measured pulse height spectra in Fig. 17.25. For relatively thin films,
the two fission fragment branches are clearly discernible. For thicker films, the energy distribution becomes
skewed towards the lower energies, a consequence of energy self-absorption for fission products that lose
energy as they transit the UO2 film before emerging into the detector gas. Because the lightest and most
energetic fission products cannot reach the detector gas if born at a distance greater than about 8.0 microns
from the coating surface, there is no practical reason to apply films any thicker. Hence, the thermal-neutron
detection efficiency for a 235 UO2 -coated detector is limited to less than about 0.5%. Fission chambers with U
metal instead of UO2 are also manufactured, and have a higher density of U per unit volume. However, the
fission product ranges in U are also shorter (less than about 6 μm) than in UO2 ; consequently, the resultant
thermal-neutron detection efficiencies are also less than about 0.5%.
One method to increase the thermal-neutron detection efficiency of fission chambers is to include in the
chamber multiple plates each of which is coated with fissile material [Lamphere 1960]. These plates are
separated by small gaps usually of about 2 to 5 mm [Bogdzel et al. 1982; Wender et al. 1993]. The chambers
are usually backfilled with Ar, often at elevated pressures to improve energy absorption of the fission products
in the small gaps. The plates are biased with opposing voltages to collect electron-ion pairs liberated in the
gas by the fission fragments.
Fission chambers deployed in a nuclear reactor suffer from burnup just as does the nuclear fuel. Over time
the amount of fissile material becomes depleted and the detector response decreases. The initial sensitivity
of a fission chamber can be increased by using enriched 235 U, but the signal rapidly diminishes with neutron
fluence and decreases to approximately half the initial response after an exposure of 1021 thermal neutrons
cm−2 [Jackson 1967]. Consequently, without periodic recalibration, the signal output no longer accurately
measures the reactor power. This problem of decreasing sensitivity can be mitigated by including fissile and
fertile materials in the fission chamber, thereby producing a type of breeder detector known as a regenerative
fission chamber. Some regenerative chambers include 235 U and 234 U [Jackson 1967], 239 Pu and 238 U [Böck
and Balcar 1975], 235 U and 238 U and natural U with 232 Th [Reichenberger et al. 2014]. With appropriate
mixing ratios of these isotopes, the signal variation can be constrained to less than 5% for neutron fluences
extending, in some cases, beyond 1022 cm−2 , which correspond to fluences accumulated over several years
in the core of a power reactor.
The build-up of fission products inside the chamber increasingly makes the chamber radioactive. Conse-
quently, a background signal from the radioactive emissions of the fission products increases with time, and
remains even after the reactor is shut down. This effect is often called the memory effect [Roux 1966]. The
amount of fission product build-up and memory current is a function of the fissile material mass, neutron
flux, and irradiation time. Consequently, the residual memory effect, as described by normalized currents,
differs among fission chamber designs. To understand the general effect of fission product build-up, Roux
[1966] describes the memory effect as a normalized current which varies with the irradiation time in a nuclear
Sec. 17.3. Gas-Filled Slow Neutron Detectors 845

Figure 17.25. Calculated and experimentally measured pulse height spectra of fission fragments from UO2
film thicknesses of 28.6 nm, 714 nm, 2.53 μm, and 7.54 μm. Data are from [Kahn et al. 1965].
846 Slow Neutron Detectors Chapt. 17

Figure 17.26. Calculated and experimental fission-chamber normalized resid-


ual currents from fission products as a function of time after irradiation. Shown
are normalized currents for varied irradiation times. Data are from [Roux
1966].

reactor and the subsequent time after irradiation (see Fig. 17.26). A few features can be observed from the
Roux results following irradiation: first within a few seconds, the memory current drops by a factor of 103 ,
and second it can take many days for the memory current to reduce by a factor of 105 .
Fission chambers can be operated in pulse-mode, current mode, and Campbelling mode. Because of the
multiple operational modes, fission chambers are often used in “wide range” channels in nuclear instrumen-
tation systems. For low flux situations, pulse mode operation offers the advantage that each interaction can
be discriminated from background. The disadvantage is that operation is restricted to lower count rates to
reduce dead time problems. Pulse mode is used mainly for start-up because it can be used to distinguish
between neutrons and gamma rays. At elevated count rates, fission chambers can be operated in current
mode, which has the advantage of no longer suffering dead time problems. The measured time-averaged
current is proportional to the average power density at the detector location. However, signals from various
radiations are no longer distinguishable. The use of Campbelling mode (or mean square voltage mode)
does assist with gamma-ray and background discrimination [Campbell and Francis 1946; Vermeeren et al.
2011]. The output signal is still a form of current mode, in which the output is a combination of signals
from steady-state and a time varying components. The Campbelling circuit is used to block the steady-state
component while squaring the time varying component. The resulting signal is proportional to the square
of the charge that is created by each incident particle of radiation, thus enhancing the difference between
types of radiation [Geslot et al. 2011]. Hence, the neutron induced portion of the signal is enhanced, while
the gamma-ray component is reduced. Thus, Campbell mode operation is useful for neutron measurements
in a high gamma-ray background.
Commercial units designed as beam port monitors may have a “pancake” design so that only a small
fraction of the neutrons passing through a sensitive volume interact and are detected. Typical diameters
of such detectors are about 70 to 115 mm. The purpose of the design is to provide an in-situ neutron
measurement of the beam intensity while minimally perturbing the beam.
Sec. 17.3. Gas-Filled Slow Neutron Detectors 847

Cylindrical detectors are fashioned generally in a coaxial-type design, but one in which the inner anode
diameter is relatively large, often having nearly the same diameter as the outer cathode. Hence, these
detectors are not designed to produce an avalanching field as occurs in common proportional counters.
The gap between the anode wall and the cathode wall is typically only a few mm. Consequently, the
device performs more as a parallel plate detector rather than a coaxial gas-filled detector (as described
in Chapters 10 and 11). Designs may have the cathode or anode coated with the fissile material. In
either case, fission fragments are ejected into the small gas volume between the cathode and anode walls
and deposit in the gas only a fraction of the total fission product energy. Elevating the gas pressure can
increase the energy deposition, although most commercial units are pressurized at only 1 atm. The fill
gas is often a combination of Ar and N2 . The argon is more effective at absorbing energy from the fission
fragments and serves as the detection gas (see Table 9.1), while the N2 has a higher electron mobility
so as to produce faster pulse rise times (see Fig. 10.10). As shown in Table 9.1, the ionization energy
for N2 is slightly less than that of argon so that charge can be transferred from ionized argon to the
nitrogen. The small gas-filled gap limits energy deposition from fission fragments and background radiations.
However, because the energy deposited in this gap by fission fragments is significantly larger than that
deposited by beta particles, gamma rays, and alpha particles, pulse height discrimination can be used to
distinguish between neutron induced events
and background.
Sub-miniature fission chambers (SMFC)
have been under development for in-core
nuclear reactor monitoring for many years
[Poujade and Lebrun 1999; Blandin et al.
2003; Lamirand et al. 2014]. These de-
tectors are manufactured with a traditional
coaxial design but with the distinction that
the outer diameter is approximately 1.5 mm.
The anode is also thicker in diameter than
that required for proportional counters and
is coated with a enriched fissile material such
as 97% 235 U [Blandin et al. 2003]. The sen-
sitive lengths of such SMFCs are approxi-
mately 1 cm. The detectors are backfilled
with Ar gas pressurized between 1 to 1.5
atm. Sub-miniature detectors are designed
to operate in high neutron fluxes in the core Figure 17.27. Pulse shape comparison of the Fuchs-Nordheim model
of a nuclear reactor with some designs now prediction and measured results from an MPFD for a $2.77 reactivity
under investigation for transient measure- insertion. The experiment was conducted in a TRIGA nuclear reactor
15 −2 −1
ments. Commercial variations of the sub- with thermal peak flux of 9.28 × 10 cm s . Data are from [Nichols
et al. 2018].
miniature design are available.
Another type of miniaturized fission chamber is the micro-pocket fission detector (MPFD). These tiny
devices are significantly smaller than normal fission chambers and have dimensions of approximately 1 mm
with gas volumes of 0.5 mm3 or less. Although the small volumes are incapable of absorbing the total energy
from any of the fission products, the amount of energy absorbed is about 3 to 7 MeV for all fission products,
regardless of the branch [McGregor et al. 2005]. The small volume ensures that background gamma-rays
and beta particles deposit less than 1 keV, too small to be detected. Alpha particle emission from the
reactive coating can deposit more energy, but also is small, typically only 60 keV or less. Hence, simple
pulse height discrimination can be used to separate neutron-induced events from the radiation background.
848 Slow Neutron Detectors Chapt. 17

MPFDs are intentionally designed to be inefficient because they are intended as in-core instrumentation for
nuclear reactors. Because of their small size, they can be inserted into tiny test ports without causing flux
perturbations. Dead time is also less of an issue, mainly because the electron-ion drift times are much smaller
for these detectors than traditional fission chambers. These detectors have been operated in pulse mode for
neutron fluxes ranging up to 1013 n cm−2 s−1 [McGregor et al. 2005].
Variants of these miniaturized fission chambers are under investigation for different reactor cores and
applications [Reichenberger et al. 2016, 2017]. One variant eliminates the need to plate fissile material on an
electrode and uses a parallel electrode wire geometry to collect the charges from the miniature gas pocket.
With reactor excursion experiments, current mode operation shows that these detectors can track reactor
excursions up to a thermal flux of at least 9.28 × 1015 n cm−2 s−1 as demonstrated in a TRIGA nuclear
reactor [Nichols et al. 2018]. When compared to the Fuchs-Nordheim model [Fuchs 1946; Nordheim 1946],
the experimental results match well to the model (see Fig. 17.27), showing experimentally a FWHM of 13.2
ms compared to the predicted value of 12.2 ms.

17.4 Scintillator Slow Neutron Detectors


Scintillators used for slow neutron detectors can be categorized into two groups, (1) those composed of a single
compound that both fluoresces and also interacts strongly with thermal neutrons and (2) those composed
of a mixture of two compounds, one of which fluoresces and the other of which contains neutron reactive
material. For instance, LiI and CLYC are in group 1, whereas boron loaded plastic and liquid scintillators
are in group 2. Some examples are briefly discussed here. Greater detail about these scintillators is provided
in Chapter 13 and also by Van Eijk et al. [2004] and Birowosuto [2007].

17.4.1 Neutron Reactive Scintillators


LiI Scintillator
LiI:Eu crystal, described in Chapter 13, is a highly hygroscopic alkali-metal halide scintillator, recognized
by Hofstadter et al. [1951] for its unique properties suitable for thermal and slow neutron detection. It has
a density of 4.076 g cm−3 and a relative molecular mass of 133.89. The natural abundance of 6 Li is 7.59%
with a 2200-m/s (n,t) cross section of 938.0 b.14 It then follows that the macroscopic (n,t) cross section for
2200-m/s neutrons is 1.31 cm−1 ; hence over 70% of thermal neutrons are absorbed in a crystal 1 cm thick.
The attenuation length can be decreased by growing LiI enriched with 6 Li. The most probable emission
wavelength λmax is approximately 475 nm. As with many Eu activated scintillators, LiI is a relatively slow
scintillator with a decay constant of 1.4 μs so that its response rate is somewhat limited. The use of Tl as
the activator introduces fluorescence with short decay times [Khan et al. 2015], although a relatively long
fluorescence component persists. Further, the light yield decreases compared to LiI:Eu with a most probable
emission wavelength λmax remaining near 475 nm for activator concentrations between 0.02% and 0.5% Tl.
Not only is LiI a good neutron absorber, the high iodine content also makes it a good gamma-ray
absorber. Consequently, LiI neutron detectors can also have a relatively high sensitivity to background
radiation counts. Because the 6 Li(n,t)4 He reaction releases 4.73 MeV, often simple pulse height analysis is
enough to distinguish between gamma-ray and neutron events. However, pulse height discrimination may
not be an adequate discrimination technique in the presence of gamma-ray energies of approximately 4 MeV
or greater, or in intense gamma-ray environments that induce pulse pile-up [Nicholson and Snelling 1955].

14 This cross section was often called the absorption cross section, a term no longer in wide usage because it includes fission
plus 16 reactions in which the neutron disappears such as (n,γ) and 15 reactions that produce positively charged reaction
product(s) such as (n,p), (n,t), (n,2α), and (n,t2α). However, here the total 2200-m/s is 938.8 b, an indication that the (n,t)
reaction is essentially the only reaction.
Sec. 17.4. Scintillator Slow Neutron Detectors 849

LiI:Eu has been reinvestigated in recent years as a compact neutron imager. LiI grown as a microcolumnar
scintillator has been developed with the impetus of using the natural fiber optic structure for light segregation
[Nagarkar et al. 2001]. Enriched to 96% in 6 LiI, crystals were grown on fiber optic substrates to promote
light propagation to a light sensing device, in this case, a charged coupled device (CCD). The LiI films were
1.2 mm thick with 30 μm diameter microcolumns. Measurements indicated that a spatial resolution of 110
μm is achievable.
LiI:Eu scintillators attached to either a Si PIN diode [Pausch and Stein 2008] or a SiPM [Foster and
Ramsden 2008] have been investigated as compact neutron detectors. The advantage of such a structure is
the lower operating voltages required and the smaller overall volume. Pausch and Stein [2008] report results
from a 3-mm-thick LiI:Eu detector exposed to a mixed gamma-ray/neutron field, in which a moderated
AmBe source and 137 Cs and 60 Co sources were used. It was found that counts from gamma-rays interacting
in the LiI scintillator or directly interacting in the semiconductor diode can be significant and, consequently,
lead to misinterpretation of gamma-ray counts as neutron counts. Pausch and Stein [2008] report a pulse
processing method that can discriminate between gamma-ray and neutron events. Foster and Ramsden
[2008] report the appearance of artifacts in the pulse height spectrum when the LiI/SiPM combination was
exposed to a mixed gamma-ray/neutron field, in which a modestly moderated 252 Cf source and a 137 Cs
source were used. It is less likely that the artifacts are from direct gamma-ray interactions in the SiPM,
mainly because the depletion region in a SiPM is relatively small (smaller than in a PIN diode). Instead, it
is hypothesized that the artifacts result from neutron scattering from Li nuclei [Foster and Ramsden 2008].
Also observed was a strong dependence of the neutron induced pulse height spectrum and the operating
temperature. Foster and Ramsden [2008] argue that the thermal dependence is of little consequence, mainly
because the pulse height spectrum is only used for a LLD setting and not for spectroscopy, and that bias
adjustments to the SiPM can help compensate thermal changes in the pulse height spectrum.

Elpasolite Scintillators
Cesium lithium yttrium chloride (Cs2 LiYCl6 or CLYC) and other elpasolites containing Li can be used for
slow neutron detection [van Eijk et al. 2005]. Lithium-based elpasolites are sensitive to both neutrons and
gamma rays, and have been used to detect both. For low count rate measurements, the relatively good energy
resolution of CLYC:Ce and also cesium lithium yttrium bromide (Cs2 LiYBr6 or CLYB) allows pulse height
discrimination (PHD) between neutron and gamma-ray counts, just as with LiI:Eu detectors. The α/β ratio
for CLYC:Ce is 0.66, an indication that pulse shape discrimination (PSD) could be used to discriminate
between gamma rays and neutrons. CLYC:Ce also possesses core valence luminescence (CVL) that produces
only a fast component from gamma-ray events. The same is not true for neutron events. Hence, PSD can
be performed by simply distinguishing between events with and without CVL. Note that the long decay
times characteristic of elpasolites can be a problem in high mixed radiation fields for either PHD or PSD,
mainly because pulse pile-up contaminates the neutron-induced spectrum. The elpasolite Cs2 LiLaBr6 (or
CLLB) has better energy resolution than CLYC:Ce [Glodo et al. 2011], but apparently lacks core valence
luminescence [Bessiere et al. 2005]. However, neutron PSD can be achieved by comparing the decay time
of the decay components (as described in Chapter 13), mainly because the slow components differ with the
radiation type, where the induced gamma-ray tail has a longer duration than the neutron induced tail.
CLYC:Ce can be obtained commercially and can be coupled to either a traditional PMT or a SiPM. Spec-
tral performance is good with approximately 4.5% FWHM for 662-keV gamma rays. It performs adequately
well for gamma-ray spectroscopy and neutron detection. However, for high energy resolution gamma-ray
spectroscopy, there are other scintillators that can outperform CLYC:Ce (such as LaBr3 ). The same is true
for compact neutron detectors. Hence, the main novelty of CLYC:Ce is the ability to detect efficiently both
gamma rays and neutrons with a single device.
850 Slow Neutron Detectors Chapt. 17

A significant disadvantage to CLYC:Ce is that both 133 Cs (100% natural abundance) and 35 Cl (75.78%
natural abundance) are moderate neutron absorbers that transmute into radioisotopes that emit beta par-
ticles. Further, their atomic ratios per molecule are much higher than Li. For natural constituents, ap-
proximately 78% of neutron absorptions in CLYC:Ce do not produce a spontaneous neutron reaction, but
rather increase the background from emissions of beta particles and gamma rays. Consequently, the intrinsic
thermal-neutron detection efficiency of CLYC:Ce is limited to approximately 22%. If natural Li is replaced
with enriched 6 Li, the thermal-neutron detection efficiency has an upper limit of 80%. To remedy this
problem, other elpasolites without Cs and Cl have been explored and a successful candidate was found to
be Rb2 LiYBr6 (or RLYB:Ce) [van Eijk et al. 2005]. Overall, the light output and performance of RLYB:Ce
is similar to CLYC:Ce although, at the time of this writing, it is not commercially available. Another in-
troduction to the elpasolite family with promising results is Cs2 LiLa(Br6−xClx ) or CLLBC:Ce, which has
good gamma-ray energy resolution along with the neutron detection characteristic of CLYC:Ce [Shirwadkar
et al. 2012]. The substitution of Br for Cl works to reduce parasitic neutron losses, while the substitution
of La for Y works to slightly increase parasitic neutron losses. CLLB:Ce has become commercially available
with reported energy resolution for 662 keV gamma rays of approximately 4% FWHM.15 The popularity of
CLLB:Ce is likely to increase in the coming years because of its dual application to neutron and gamma-ray
detection.

LGBO Scintillator
Many other scintillators with reactive components have been investigated. For instance, Li6 Gd(BO3 )3 :Ce
scintillators with varying concentrations of Gd, B, or Li enrichments have been studied [Czirr et al. 1999].
Li6 Gd(BO3 )3 :Ce can be produced as a powder or as a transparent crystal [Czirr et al. 1999]. Three of
the main constituents react with neutrons, namely, 6 Li(n,t)4 He, 10 B(n,α)7 Li, and 155,157 Gd(n,γ)156,158 Gd.
The neutron absorption response of this interesting scintillator can be changed by adjusting the ratios of
the neutron absorbing nuclides to their non-reactive isotopes. When using materials of natural abundance,
the Gd component dominates neutron absorption. Consequently, the reaction products are mainly gamma-
rays and low energy conversion electrons, and the Li and B components contribute little to the response.
Recapture of the gamma rays is inefficient and the conversion electrons have short ranges, a property which
unfortunately limits the response. Van Eijk [2001] reports that natural Li6 Gd(BO3 )3 :Ce produces a low-end
average light yield of 14,000 photons/neutron. Note that this average is a compilation of three uniquely
different emissions from the four possible reactions. According to Czirr et al. [1999], light emission ratios for
Gd, B, and Li per neutron are approximately 2, 11, and 52, respectively. In these results the representative
conversion electron energy of 85 keV has been substituted for the Gd emissions (see Schulte et al. [1994]).
Hence, the pulse height from 6 Li(n,t)4 He is significantly higher than those from other reactions.
If the Gd is depleted of 155 Gd and 157 Gd, then the boron component can dominate the absorption. If the
10
B is then also omitted, the Li component dominates neutron absorption even further. Czirr et al. [1999]
conclude that a good compromise is to produce 6 Li6 [nat−(155,157)] Gd(11 BO3 )3 :Ce so as to take advantage
of the high energy reaction products from 6 Li and the resultant light yield of 56,900 photons/neutron.
The reaction product ranges, and subsequent light attenuation lengths, are still problematic in a manner
similar to that for coated gas-filled detectors. In an attempt to overcome this problem, Allier [2001a, 2001b]
suggest Si diode well-structures backfilled with Li6 Gd(BO3 )3 :Ce powder. In summary, Van Eijk [2001]
notes that advantages include the low index of refraction of 1.66 and the high neutron absorption efficiency.
Disadvantages include the longer decay times that range from 200 ns to 800 ns and the high cost of Gd
depleted of 155 Gd and 157 Gd.

15 Through Saint-Gobain Crystals.


Sec. 17.4. Scintillator Slow Neutron Detectors 851

GSO Scintillator
Gadolinium orthosilicate (Gd2 SiO5 :Ce or GSO) is another gadolinium-based scintillator that has been studied
as a possible neutron detector [Reeder 1994a, 1994b; Uozumi et al. 1997]. This scintillator has a fast decay
component (56 ns) that is responsible for 85-90% of the light yields and a slow component (600 ns) that
is responsible for the remaining 10-15% of the light yield [Melcher et al. 1990]. The maximum wavelength
is 430 nm and matches well to bialkali PMTs. However, the light yield is relatively low at only 12,500
photons/MeV. Reeder [1994a] notes that the pulse height spectrum peak is approximately 77 keV equivalent
and matches well to the Gd conversion electron spectrum [Schulte et al. 1994]. Because GSO is sensitive to
both gamma-rays and neutrons, it can be used to detect both. Reeder [1994a] lists advantages of GSO as
simplistic because it has dual detection capabilities as well as compact and efficient because a small crystal
readily absorbs neutrons. Disadvantages include competition between low-energy background gamma rays
and the Gd conversion electron emissions as well as contamination by characteristic x-rays from the shielding
(especially from Pb).
Because conversion electrons, Compton electrons, and photoelectrons produced by neutrons and gamma
rays have fundamentally similar properties, discriminating between neutron and gamma-ray events with
pulse shape discrimination does not appear to be an option [Uozumi et al. 1997]. Further, the complex
nature of the combined spectra makes simple pulse height discrimination difficult. Reeder [1994b] attempts
to address this problem by coupling thin GSO crystals to PMTs, so thin that the probability of gamma-ray
interactions is significantly reduced below that of thermal-neutron absorptions, all the while retaining the
ability to capture the conversion electron reaction product emissions. To demonstrate the concept, Reeder
[1994b] compared the response of a 60 μm thick GSO crystal and a 1 cm thick GSO crystal to gamma-
ray and neutron emissions from a moderated PuBe source, as well as gamma-ray emissions from a 137 Cs
source. Although the work qualitatively demonstrates the concept, the sample areas (and solid angles) were
different, thereby making quantitative conclusions difficult. Regardless, it is clear that thick crystals of GSO
neccessarily have problems with background gamma rays interfering with the neutron-induced pulse height
spectrum.
LiBaF3 Scintillator
The scintillator LiBaF3 has also been studied as a neutron detector [Knitel et al. 1996; Combes et al.
1998]. LiBaF3 has multiple emission wavelengths with different decay times, ranging from 1 ns up to 13
μs depending on the doping type and concentration [van Eijk 2001]. The light yields and decay times are
significantly different for gamma-ray and neutron interactions. A bright fast component is produced by
gamma-ray interactions (about 1,200 photons/MeV with a mean lifetime τ of about 0.8 ns), which is absent
for neutron interactions [Knitel et al. 1996]. A method that rejects these high amplitude fast pulses is used
to discern between neutron and gamma-ray events [Knitel et al. 1996; Combes et al. 1998]. Van Eijk [2001]
argues that the fast emission produced by gamma-ray interactions is due to core-valence luminescence, which
is accompanied by the delayed luminescence from self-trapped holes. The fast core-valence luminescence is
altogether missing for neutron interactions. Combes et al. [1998] report that the use of radiation damaged
LiBaF3 crystals have improved discrimination between gamma-ray and neutron events. Along with co-doping
with Ce and Rb, the damaged material produced a fast decay time for the self-trapped hole luminescence,
thereby reducing issues with pulse pile-up while improving the signal to noise ratio [Combes et al. 1998].

17.4.2 Scintillators Loaded with Neutron Reactive Materials


Organic Scintillators
Organic scintillators loaded with either 10 B, 6 Li, or natural Gd are commercially available as neutron detec-
tors. These materials are usually applied to fast neutron measurements, but can also be used for thermal
or slow neutron detection. The concept is simple; neutrons are absorbed in the absorber, either 10 B or 6 Li,
852 Slow Neutron Detectors Chapt. 17

which release energetic reaction products that subsequently cause fluorescence in the scintillator. These de-
tectors can be economically manufactured in large sizes and formed into multiple shapes. The light emission
can be significant, mainly because of the high Q-values from the 10 B(n,α)7 Li and 6 Li(n,t)4 He reactions.
The amount of boron that can be loaded into an organic plastic scintillator (polyvinyltoluene) is limited
by the reduction in scintillator transparency. Loading is usually no more than 5% by weight for commer-
cial boron-loaded organic scintillators, and these scintillators have lower light yields than their unloaded
counterparts by approximately 20% [Drake et al. 1986] (see also Table 13.2). Commercial plastic scintilla-
tors, such as EJ-254 and BC-454, are loaded with natural boron; hence, the actual 10 B loading amounts
to approximately 1%. Higher boron loadings are available by special request. Although the Q-value of the
boron reaction is high, in Chapter 13 it was mentioned that light yield in organic scintillators is lower for
heavy ions than for electrons. The work of Verbinski et al. [1968] can be used to find an approximate light
yield for the 10 B(n,α)7 Li reactions products compared to energetic electrons. For instance, the scintillation
signals from 10 B(n,α)7 Li reactions are approximately equivalent to that of 76-keV electrons [Drake et al.
1986; Eljen 2016a]. Consequently, gamma-ray background can interfere with neutron measurements. For
fast neutrons, the initial (n,p) reaction in the plastic produces a prompt light response, followed by a time
delay of approximately 2.7 μs before the light response from a 10 B(n,α)7 Li reaction appears. By measuring
both light emission pulses from the proton recoil and the subsequent 10 B(n,α)7 Li reaction products, fast
neutron interactions can be readily identified [Drake et al. 1986].
Liquid Scintillators
Liquid scintillators loaded with neutron reactive absorbers are also commercially available, and, in many
ways, are more attractive as slow neutron detectors than are plastic scintillators. For liquid scintillators
loaded with boron, pulse shape discrimination methods can be used to distinguish between gamma-ray and
neutron events [Chou and Horng 1993]. Commercial products are available loaded with either natural or 90%
enriched 10 B. Loading is typically 5% by weight, which yields 1% 10 B loading by weight for natural boron
and 4.6% 10 B loading by weight for fully enriched boron. A variety of loadings can be obtained by special
request. For electron and gamma-ray events, the light yield is approximately 65% that of anthracene, which
is similar to that of other organic scintillators. The pulse height from a 10 B(n,α)7 Li event is approximately
equivalent to a 90-keV electron pulse [Eljen 2016b]. For fast neutrons, the average capture time is a function
of the 10 B loading, ranging from 0.3 μs for 5% enriched 10 B loading to 1.4 μs for 5% natural boron loading.
Also, there is on average a 2.7 μs delay between the initial (n,p) reaction emission and the 10 B(n,α)7 Li
emission, a delay which permits neutron identification with delayed time gating methods.
Liquid scintillators loaded with natural Gd rely on prompt gamma rays and conversion electron emis-
sions from the 157 Gd(n,γ)158 Gd and 155 Gd(n,γ)156 Gd reactions. These scintillators are used for neutron
spectroscopy and neutrino detection. Gd loading for commercial products is typically 0.5% by weight, but
special Gd concentrations are available.
Because liquid scintillators are often employed in large containers, the solvents are chosen to have high
flash points to reduce the risk of combustion.16 Also, liquid scintillators can be contaminated with water
moisture, a condition that compromises performance. Hence, the user must take care to keep exposure to
air at a minimum. Typically these liquid scintillators are packaged under an inert environment (gas).
Ceramic Neutron Sensitive Scintillators
Li Glass Scintillators Cerium activated silicate glasses were introduced in the late 1950s for radiation detec-
tion [Ginther and Schulman 1958]. Although boron loaded glasses were also investigated for neutron detection
[Bollinger et al. 1959], it is the Li-loaded class of silicate glasses [Voitovetskii et al. 1960a, Voitovetskii and

16 The flash point of a liquid is the temperature at which the liquid has sufficient vapor pressure in equilibrium with the liquid
to just form a flammable atmosphere.
Sec. 17.4. Scintillator Slow Neutron Detectors 853

Table 17.2. Properties of Ce activated 6 Li-Glass (nat. Li/ 95% enriched 6 Li/ 99.99% enriched 7 Li).

Property GS1/GS2/GS3 GS10/GS20/GS30 KG1/KG2/KG3

Total Li by weight 2.4% 6.6% 7.5%


Density g cm−3 2.66 2.5 2.42
Refractive index 1.58 1.55 1.57
Melting point (K) 1475 1475 1475
Max emission λ (nm) 395 395 395
Relative Light Yield* 22%–34% 20%– 30% 20%
Decay times, neutron (ns)** 21, 69, 115 18, 57, 98 18, 62, 93
Decay times, alpha (ns)** 20, 65, 106 16, 49, 78 15, 45, 56
Decay times, beta (ns)** 21, 62, 114 20, 58, 105 17, 51, 96
Available thickness (mm) 0.1–10 0.1–10 0.1–10
Resolution of peak for
moderated PoBe neutrons 13%–22% 15%–28% 20%–30%
Linear attenuation coefficient
for thermal neutrons (cm−1 ) 0.393/4.95/0.0002 1.016/12.79/0.0006 1.118/14.07/0.0007

*Relative to anthracene.
**Fast component, slow component, 90%–10%, respectively. Data for GS2, GS20, and KG2 glasses only.

Tolmacheva 1960b; Ginther 1960; Bollinger et al. 1962] that have been researched and widely commercialized
for neutron detection. The scintillation mechanisms and properties of glass scintillators were briefly covered
in Sec. 13.2.3, with more details on the properties of Li-loaded Ce-activated silicate glasses detailed in the
literature [Spowart 1976, 1977; Fairley and Spowart 1978].
Li-loaded glass scintillators, activated with Ce, are commercially available in a variety of concentrations
and enrichments, as summarized Table 17.2.17 The absorption characteristics of such glasses are shown in
Fig. 17.28. These glass scintillators can be obtained in various sizes, thicknesses, and 6 Li doping concentra-
tions. Perhaps the most common of the Li glass materials used by commercial instrumentation companies
is GS20 with 6.6% doping of 95% enriched 6 Li. GS20 has a maximum emission wavelength of 395 nm with
between 20% and 30% of the light yield compared to that of anthracene. The light yield for GS20 glass
ranges between 3,270 photons/MeV to 5,550 photons/MeV, depending upon the glass thickness and scintil-
lation yield standard. For full energy absorption within the scintillator, the total light yield per interaction
ranges between 15,450 and 26,200 photons/MeV centered about a wavelength of 395 nm. There are other
Li glasses available, with a general labeling convention in which ‘1’ designates natural lithium, ‘2’ designates
95% enriched 6 Li, and ‘3’ designates 99.99% enriched with 7 Li, which is insensitive to neutrons.
The decay constants are a function of radiation type and the Li loading, and generally have fast and
slow decay components [Fairley and Spowart 1978]. Yet, from Table 17.2, these decay times vary only small
amounts between radition types. There are varied Li loadings, with commercial codes [Spowart 1976, 1977]
listed as 2.4% (GS1,GS2,GS3), 6.6% (GS10,GS20,GS30) and 7.5% (KG1,KG2,KG3) by weight. The ranges
of the 6 Li(n,t)4 He reaction products in Li glass, tritons and α particles, are approximately 36.3 microns
and 6.3 microns, respectively. Absorptions near the glass surface can lead to reaction products escaping the
scintillator and decreasing the light output, an effect known as the “edge effect” [Yamaguchi 1989]. This
situation can be remedied by fastening sheets of 7 Li-glass, such as GS3, GS30, or KG3, that is depleted of 6 Li

17 The traditional designations for the different Li glass scintillators come from Levy West Laboratories, which became Applied
Scintillation Technologies and is now named Scintacor. The ‘GS’ designation is, presumably, named for Ginther and Schulman.
854 Slow Neutron Detectors Chapt. 17

Figure 17.28. Absorption characteristics of 2200 m s−1 neutrons in various


Ce activated Li glasses.

to 99.99% on both sides of the neutron sensitive Li glass. Reaction products escaping the neutron sensitive
region fluoresce the 7 Li-glass and, thus, allow emitted photons to be recovered. Lithium glasses provide a
convenient way to produce large area sheets of a neutron scintillator and are used to detect both thermal
and fast neutrons. They can be used under high pressure and at high temperatures because of their high
melting point of 1475 K. Spowart [1977] reports a luminescent thermal dependence that reaches a maximum
near 450 K, reducing with either higher or lower temperatures.

Gadolinium Oxysulfide Ceramics Gadolinium oxysulfide (Gd2 O2 S, GOS or Gadox) is used for thin scin-
tillator screens. It is available as a powder, but can be hot pressed into a translucent ceramic [Greskovich
and Duclos 1997]. Co-dopants include Pr, Ce, and F, and have a central emission wavelength of 580 nm
and emit 40,000 photons/MeV [Lecoq et al. 2006]. The emission decay time is relatively long at 2.1 μs.
Gadox is primarily used for digital radiography imaging panels for x-ray excitations. However, its elemental
Gd constituent produces a high neutron absorption efficiency; hence, it has been evaluated as a neutron
scintillator. Because Gd is a good absorber of photons and neutrons, and the resulting reaction products
are nearly indistinguishable (Compton electrons, photoelectrons, conversion electrons), there are difficulties
in distinguishing between neutron and background gamma-ray events.
nat
However, because Gd is such a strong thermal-neutron absorber (σGd (n,γ) = 48, 610 b at 2200 m/s),
only a thin layer is necessary for adequate performance. For instance, the density of Gadox is 7.34 g cm−3
with a corresponding 2200-m/s macrocroscopic cross section of 1,360 cm−1 . These values indicate that a
layer only 10 μm thick absorbs over 85% of intersecting thermal neutrons. Lindsay et al. [1986] report the
use of a thin layer of Gadox on a LIXI (Light Intensifier X-ray Image) scope, in which the background
Sec. 17.5. Semiconductor Slow Neutron Detectors 855

from gamma-ray interactions is suppressed for real-time neutron radiography. Kardilov et al. [2011] report
methods to improve performance of Gadox films for neutron imaging by imbedding the scintillator in sodium
silicate (or “water glass”) and applying an Al reflective coating. Greskovich and Duclos [1997] report that
the hexagonal crystal structure of Gadox limits light collection, a consequence of optical anisotropy, residual
porosity, and foreign phases from densification additives. They also report that Gadox is susceptible to x-ray
damage, more so than many other ceramic scintillators.

Zinc Sulfide Scintillator Zinc sulfide activated with silver is a bright scintillator (see Chapter 13) with
a light yield that is approximately 130% of that of NaI:Tl. This material is often mixed with neutron
reactive materials to produce a thermal-neutron detector. For instance, LiF or B2 O3 mixed with ZnS:Ag
make effective scintillating films. ZnS:Ag is available mainly in powder form, and it is also opaque to its
own light emissions, a property that limits the working thickness of the material to no more than 25 mg
cm−2 or about 60 microns. The most probable light emission wavelength is centered at 450 nm and matches
adequately well to most PMTs. The index of refraction is 2.36 at 450 nm that can become a significant
source of internal reflection if coupled directly to glass or PMMA (θc = 39.5 ◦ ). ZnS:Ag is often (incorrectly)
stated to be insensitive to gamma rays and beta particles. Actually, ZnS:Ag is sensitive to both gamma
rays and electrons; however, the amount of energy deposited in a thin film of only 60 microns or less by an
energetic electron is relatively small and easily distinguished from heavy ion reaction products from either
6
Li(n,t)4 He or 10 B(n,α)7 Li by pulse height discrimination.

17.5 Semiconductor Slow Neutron Detectors


Semiconductor slow-neutron detectors can be classified as either coated detectors or bulk detectors. Coated
detectors are electron devices, usually Schottky or junction diodes, upon which a neutron reactive coating
has been applied. Bulk detectors are semiconductors with one or more neutron reactive constituent isotopes.
There are variations of both types [Caruso 2010], and a few of the more important structures are described
below.

Coated Semiconductor Neutron Detectors


Coated semiconductor neutron detectors are generally Neutron
fashioned as semiconductor diodes with a neutron re- Converter
SiO2
active coating applied to the rectifying contact.18 The Isolation
first such detector was a small Si pn junction diode, only
a few square milimeters in area, with a 10 B film vapor
deposited upon the rectifying junction [Babcock et al. Blocking - ++
Contact Reaction - +
1959]. Although studied for decades, these coated semi- Products - Metal
Contacts
conductor neutron detectors were viewed as novel de- Ohmic
Contact Semiconductor
vices for dosimeter packages, primarily because of their
inherently low efficiencies. However, recently, with the
introduction of microstructured semiconductor neutron Figure 17.29. The basic construction of a coated planar
detectors (MSNDs), they are receiving renewed atten- semiconductor diode neutron detector.
tion because of their high neutron detection efficiencies. Overall, there are two main types of coated semi-
conductor neutron detectors, namely planar diode detectors and MSNDs.

18 Insome of the original literature on these devices, they are called “foil detectors” because a thin foil of the neutron reactive
material was positioned adjacent to the semiconductor diode detector. However, almost all detectors of this sort now have the
reactive material applied directly to the rectifying junction of the semiconductor diode; hence, “foil detector” is no longer a
suitable description.
856 Slow Neutron Detectors Chapt. 17

Planar Diodes Thin film neutron detectors consist of semiconductor diodes, preferably with relatively
thin contact layers, upon which a layer (or layers) of neutron reactive material has been deposited. The
basic concept has been used by a variety of research groups (see the review by Caruso [2010]). As shown
in Fig. 17.29, neutrons absorbed in the neutron reactive film release charged-particle reaction products in
opposite directions, one of which may enter the semiconductor diode detector. Charged particles entering the
detector lose their energy through Coulombic scattering, thereby creating a high density cloud of columnar
ionization in the form of electron-hole pairs. The semiconductor diode detector is voltage biased to separate
the electron-hole pairs and drift the charges to their respective contacts. The mobile charges each induce
an image charge on the contacts as they move through the device, and the induced charge is integrated and
measured by an external preamplifier and accompanying electronics. The basic structure of a planar coated
semiconductor neutron detector is depicted in Fig. 17.29 that shows neutron reactive material fastened to the
electrical contact adjacent to the diode rectifying contact. Advantages of these detectors include a compact
size and low operating voltages and, thus, make possible the production of compact neutron dosimeters
[Aoyama et al. 1992; Sasaki et al. 1998; Ndoye et al. 1999] and compact fieldable instrumentation [Schulte
and Kesselman 1999]. It is also possible to integrate multiple detectors into an array upon a single substrate
to create compact linear neutron imaging arrays [Campbell et al. 1997; Schelten et al. 1997; Petrillo et al.
1999; McGregor 2002b] or 2-dimensional neutron imaging arrays [Mirashghi et al. 1992, 1994; McGregor et
al. 1996b; Unruh et al. 2009].
Semiconductor diodes coated with a neutron reactive material have been studied as neutron detectors
for well over fifty years and date to the original work by Babcock et al. [1959]. Most of the devices reported
in the literature either have a coating of 10 B [Rose 1967] or 6 LiF [Pospı́s̆il et al. 1993], although Gd [Feigl
and Rauch 1968] and pure Li metal coatings [McGregor et al. 2003] have also been explored. Si is the
semiconductor substrate most often used as the substrate, mainly because it is relatively inexpensive and
has a small thermal-neutron interaction cross section of σ(n,γ) = 0.17 b. However, gallium arsenide (GaAs)
[McGregor et al. 2000] and chemical vapor deposited (CVD) diamond [Foulon et al. 1998] have also been
explored as semiconductor substrates for coated neutron detectors. Simple semiconductor diodes coated

Figure 17.30. (left) Thermal neutron (2200 m s−1 ) detection efficiency vs. film thickness for front
and back irradiation of a Si detector coated with 10 B or 6 LiF. (right) Thermal neutron (2200 m s−1 )
detection efficiency vs. film thickness for front and back irradiation of a Si detector coated with 6 Li
metal. [from McGregor et al. 2003].

with either 10 B or 6 LiF are limited to approximately 5% thermal-neutron detection efficiency [McGregor et
al. 2003], and consequently have received limited application as neutron detectors. Detectors can be stacked
in various configurations to improve efficiency [McGregor et al. 2003], similar to stacking gas-filled neutron
detectors. The same equations, Eqs. (17.34) to (17.38), used to calculate efficiencies for coated gas-filled
Sec. 17.5. Semiconductor Slow Neutron Detectors 857

neutron p-type
6
LiF contact
43.4 um

SiO2 34.5 um

isolation 25.7 um

492 um
Au contacts

n-type
contact
n-type Si

Figure 17.31. (left) The basic structure of an MSND. (right) An MSND with 492 μm deep trenches,
each 25.7 μm wide, backfilled with 6 LiF nanoparticles. The Si fins are 34.5 μm wide. [from McGregor
et al. 2013b; McGregor et al. 2015].

detectors also apply to coated-semiconductor detectors, the results of which are shown in Fig. 17.30. The
efficiency can be improved by using pure 6 Li metal, in which the thermal neutron detection efficiency can
be increased above 13% [McGregor et al. 2003]. However, pure Li metal is reactive and requires moisture
proof encapsulation in an inert environment. Semiconductor detectors coated with natural Gd have also
been explored [Feigl and Rauch 1968; Schulte et al. 1994; Schulte and Kesselman 1999]. The appeal of
using Gd is because of its large thermal-neutron (n,γ) cross section of 48,610 b, but the resulting low-energy
conversion-electron and gamma-ray emissions can be difficult to distinguish from background gamma rays
in a high radiation field. A compensated detector design can help discern between background gamma rays
and neutron signals [McGregor et al. 2002b].

Microstructured Diodes Muminov and Tsvang [1987] suggested that channels etched in a semiconductor
substrate backfilled with neutron reactive material might increase the neutron detection efficiency. The
first such device was reported by McGregor et al. [2002a], and consisted of an array of holes etched into a
GaAs substrate backfilled with enriched 10 B nanoparticles. Although these initial detectors exhibited modest
efficiencies, they indicated the technology of etching microstructures into the semiconductor held promise.
Since that time, these Microstructured Semiconductor Neutron Detectors (MSNDs) have matured into a
highly efficient and compact type of neutron detector.
The basic MSND has microcavity features extending into a semiconductor surface. Within and around
the microstructures is a rectifying contact [McGregor et al. 2013b]. Many of the first generation devices had
simple Schottky barrier rectifying contacts; however, almost all recent generation devices have p-type contacts
diffused into high-resistivity n-type Si. Although the first such detectors were backfilled with enriched 10 B,
the relatively higher energy reaction-products from the 6 Li(n,t)4 He reaction produces improved detection
efficiency with better gamma-ray discrimination [Uher et al. 2007; Shultis and McGregor 2009].
Hence, modern MSNDs are mostly constructed with nanoparticles of enriched 6 LiF backfilled into the Si
microstructures. The detector configuration and operation are depicted in Fig. 17.31 (left). Neutrons interact
in the 6 LiF material, which has a macroscopic thermal-neutron (n,α) cross section of 57.4 cm−1 . Absorption
of a neutron causes the compound nucleus 7 Li* to decay into an alpha particle with kinetic energy of 2.06
MeV and a triton with kinetic energy of 2.73 MeV. For thermal neutrons, these reaction products are emitted
in opposite directions. With narrow channels, the probability of one or more reaction products emerging
from the 6 LiF absorber into the adjacent semiconductor can be relatively high. Those reaction products that
do enter the semiconductor produce a dense cloud of electron-hole pairs. An applied reverse bias across the
detector junction drifts the released electrons and holes to the electrical contacts, which induces a current
to flow, and ultimately produces a voltage pulse in the attached preamplifier circuitry. Deep channels, on
the order of 400–500 microns, increase the neutron absorption probability. Narrow channels, on the order
858 Slow Neutron Detectors Chapt. 17

of 20 microns wide, improve the probability of capturing and measuring a reaction product in the adjacent
semiconductor. The width of the semiconductor region between channels is also generally close to the channel
width of about 20 microns.
These microstructured detectors are manufactured with VLSI methods, methods which permit mass
production and, thereby lower the cost of the detectors. Si is the preferred substrate, mainly because it
has a low neutron interaction cross section and it is inexpensive. Further, the (110) orientation of Si can be
easily and rapidly anisotropically etched to form deep narrow trenches on the order of 450 microns (Fig. 17.31
(right)). The pn junction contacts are formed with traditional dopant diffusion in high-temperature furnaces,
and metallization is applied with physical vapor deposition. The backfilling of the neutron reactive material
is economically and rapidly performed by using a centrifuge to push 6 LiF nanoparticles in solution into
the channels. These detectors are fabricated on the wafer scale, yielding up to fifty 1-cm2 detectors on a
single 100-mm diameter wafer. MSNDs also require little to no applied voltage, mainly because of the deep
depletion region in the high purity Si.
In recent years, MSNDs have been fabricated as dual sided devices, with p-type regions on both sides of
a high purity n-type substrate [Fronk et al. 2015]. Neutrons that stream through the Si regions on one side
of the device encounter the neutron absorber on the other side of the device. The manufacture processing
for dual-sided MSNDs is actually easier than the singled-sided design, mainly because there is only one
diffusion step [Fronk et al. 2015]. Ochs et al. [2019] explain that the optimum packing fraction of 6 LiF in the
trenches is approximately 65% rather than solid, a consequence of the combined effects of neutron absorption
lengths and reaction product ranges. These new detectors have reached over 69% thermal-neutron detection
efficiency tn , and theoretical models suggest that values of tn up to 80% are possible [Ochs et al. 2019].
Both single and dual-sided MSNDs are commercially available, routinely fabricated with tn > 30% and
tn > 60%, respectively.19 The detectors are mass produced in compact packages as either 1-cm2 or 4-cm2
detectors.
MSNDs have several advantages as alternative neutron detectors. They are rugged and compact, and
require less than 2 volts to operate. Under certain conditions, no voltage is required to operate the detector
(although it is still required for the coupling electronics). MSNDs are relatively gamma-ray insensitive, with
discrimination ratios n/γ greater than 106 . Because MSNDs are mass produced, they can be purchased
inexpensively compared to 3 He detectors. They can be arranged in arrays with several different form factors
[McGregor et al. 2005], or can be used as single detectors for neutron dosimetry and remote neutron moni-
toring. The detectors can also be arranged in arrays with form factors of common 3 He gas-filled detectors.
A device loaded with single-sided MSNDs, having similar dimensions of a 4-atm 3 He gas-filled detector,
matched the performance of the much more expensive detector [McGregor et al. 2015]. Work with an array
of dual-sided MSNDs yielded greater efficiency than a compact 6-atm 3 He gas-filled detector of the same size
[Ochs et al. 2017], and calculations show that MSNDs can also give comparable performance to small 10-
atm 3 He gas-filled detectors. Large arrays of MSNDs arranged in blocks of HDPE have been demonstrated
as a system to locate and identify fast neutrons sources [Hoshor et al. 2015]. From the average detection
location in the 3D array of detectors, an algorithm determines the most probable type of source producing
the neutron field as well as the direction of the source.
There are reports of MSNDs with boron backfilling instead of LiF [Nikolic et al. 2008; Huang et al. 2014].
The single advantage to using boron backfilling is the higher neutron absorption cross section, thereby
reducing the mean absorption length of 180 microns for 6 LiF to only 20 microns for pure 10 B. Hence, the
microstructures can be 9 times shallower for the boron-filled device than the 6 LiF-filled device and produce
similar absorption efficiency, provided that the backfilling densities are similar. However, because the reaction
product energies and ranges are much less for 10 B than 6 LiF, there are disadvantages to the use of boron

19 Through Radiation Detection Technologies, Inc.


Sec. 17.5. Semiconductor Slow Neutron Detectors 859

[Shultis and McGregor 2009]. These disadvantages include relatively high energy loss from dead layers at
the microstructure boundaries, significant count losses from the wall effect, and the requirement of much
smaller features to etch and subsequently backfill (about 2 microns for 10 B opposed to about 25 microns for
6
LiF). Nikolic et al. [2008] have produced MSNDs as“pillar” detectors while Huang et al. [2014] report Si
detectors with holes backfilled with boron. Wu et al. [2017] have adopted the single-sided straight trench
structure for boron-filled MSNDs, reporting 32% thermal neutron detection efficiency for small devices.

17.5.1 Bulk Semiconductor Neutron Detectors


Semiconductor detectors, in which one of more constituent atoms are neutron reactive, are called bulk
semiconductor neutron detectors.20 The obvious advantages of a solid state version of a gas-filled ion chamber
is that they should have high-efficiency and a compact form. Bulk solid-state neutron detectors can be divided
into two basic categories: those that rely on the detection of charged particle reaction products and those
that rely on prompt capture gamma rays. In general, this type of neutron detector is difficult to make reliably
and at the time of writing this book is not commercially available. However, for the sake of completeness, a
brief discussion of this class of detectors is included.
The bulk materials that rely upon charged particle emissions are based on boron and lithium containing
semiconductors. In the search for bulk semiconductor neutron detectors, the boron-based materials, such
as BP, BAs, BN, and B4 C, have been investigated more than other potential materials. See, for example,
Ananthanarayanan et al. [1974], Kumashiro et al. [1987], Emin and Aselage [2005], Caruso et al. [2006],
McGregor et al. [2008], and Doan et al. [2015]. Boron-based semiconductors in cubic form are difficult to
grow as bulk crystals, mainly because they require high temperatures and high pressure for synthesis. BP
and BAs can decompose into undesirable crystal structures (cubic to icosahedral form) unless synthesized
under high pressure. B4 C also forms icosahedral units in a rhombohedral crystal structure [Clark and Hoard
1943], an undesirable transformation because the icosahedral structure has relatively poor charge collection
properties [Domnich et al. 2011] which make these icosahedral forms unsuitable for neutron detection.
BN can be formed as either simple hexagonal, cubic (zincblende) or wurtzite crystals, depending on
the growth temperature, and it is usually grown by thin film methods. It is the simple hexagonal form of
BN that has been most studied as a neutron detector. Thin film chemical vapor deposition methods are
usually employed to produce BP, BAs, BN, or B4 C. These boron-based films are often grown upon n-type
Si substrates, which can form a pn junction with the Si and, therefore, produce a simple coated Si diode as
described at the beginning of this section. Consequently, the neutron response from the device can be easily
mistaken as a bulk response when it is actually a coated diode response. To date, there is sparse evidence
of boron-based semiconductors producing intrinsic neutron signals.21
Li-containing semiconductors, categorized as Nowotny-Juza compounds, have also been investigated as
bulk neutron detectors. The Nowotny-Juza compound LiZnAs has been demonstrated as a neutron detector
[Montag et al. 2016]; however, the material is difficult and expensive to synthesize, and only small semicon-
ductor crystals have been reported. Traditional semiconductor materials with neutron reactive dopants have
been investigated, namely, Si(Li) detectors. Neutrons interact with the lithium dopant in the material and
produce energetic reaction products. However, the dopant concentration is relatively low in Li drifted Si
detectors (or other doped semiconductors), typically less than 1019 cm−3 . For a degenerate concentration of
Li on the order of 1019 cm−3 , a 5-cm-thick block of natural Si(Li) would have less than 1% thermal-neutron

20 The expression “solid-form” semiconductor neutron detectors has been used in the past by the authors, but it seems awkward
and has thus been abandoned.
21 The spectral output from many of these boron-based semiconductors grown on Si is often later identified correctly as the

spectrum from a boron-coated diode as in Fig. 17.17 [McGregor and Shultis 2004; 2005]. Films grown on insulating substrates
also may produce signals from reaction products ionizing the surrounding air.
860 Slow Neutron Detectors Chapt. 17

detection efficiency, while a 5-cm-thick block of a Si(6 Li) detector would have only 4.6% thermal-neutron
detection efficiency.
Another material currently being studied as a bulk semiconductor neutron detector is lithium indium
diselenide (LiInSe2 ) [Tupitsyn et al. 2012]. Originally studied for its optical properties [Isaenko et al. 2002],
LiInSe2 has garnered interest for its semiconductor properties. With a bandgap of 2.85 eV, the material
can operate as a room temperature detector. LiInSe2 detectors rely on the 6 Li(n,t)4 He reaction as the
neutron detection mechanism. Energy from these heavy ion reaction products is easily absorbed provided
the crystal is reasonably thicker than the combined ion ranges (that are about 80 μm). Lukosi et al. [2016,
2017] demonstrated that LiInSe2 could be used as a neutron detector and a neutron imager. Although there
appear to still be problems with producing uniform LiInSe2 crystals, this relatively new neutron detector
material shows promise. The relatively high Z value of In suggests that gamma-ray background could be
a potential problem; however, pulse height discrimination can help distinguish between gamma rays and
neutrons because of the high 4.67-MeV Q-value of the 6 Li(n,t)4 He reaction.
The mass density of LiInSe2 is 4.25 g cm−3 and the atom density is 9.15×1021 cm−3 . The resulting 2200-
m/s macroscopic cross section for the 6 Li(n,t)4 He reaction is 0.653 cm−1 . If 95% enriched 6 Li is substituted,
the 2200-m/s macroscopic absorption cross section for the 6 Li(n,t)4 He reaction increases to 8.18 cm−1 .
The indium in the compound, and to a lesser extent the selenium, combine to parasitically absorb neutrons
without producing a useful signal. Consequently, the total 2200-m/s macroscopic absorption cross sections for
natural and enriched forms of LiInSe2 are 2.64 cm−1 and 10.17 cm−1 , respectively. The combined absorption
cross sections of the various elements yield a limiting 2200-m/s neutron detection efficiency of 24.6% from the
6
Li(n,t)4 He reaction. Also, the activation of 115 In leads to the gradual buildup of a background beta-particle
and gamma-ray signal, which decays with a half-life of 54.2 minutes after irradiation. If 95% enriched 6 Li
is substituted, the limiting thermal neutron detection efficiency from the 6 Li(n,t)4 He reaction increases to
80.4%.
Prompt gamma-ray emitting semiconductors, such as CdTe [Vradii et al. 1977], CdZnTe [McGregor et al.
1996a], and HgI2 [Beyerle and Hull 1987; Bell et al. 2004], have been successfully used as neutron detectors.
Both natural Cd and Hg have relatively large thermal-neutron (n,γ) cross sections of 2444 b and 370 b
for 2200 m s−1 neutrons, respectively. These detectors rely upon the prompt gamma-ray emissions from
the 113 Cd(n,γ)114 Cd reaction (producing 558.6-keV and 651.3-keV gamma rays) and the 199 Hg(n,γ)200 Hg
reaction (producing 368.1-keV and 661.1-keV gamma rays). Because the emissions can be reabsorbed at
distances relatively far from the neutron interaction, the spatial information of the original neutron interac-
tion is lost. These semiconductor materials and detectors are best used as gamma-ray spectrometers and,
hence, are intrinsically sensitive to the gamma-ray background. The effective neutron detection efficiency is
compromised because of the relatively small Compton ratio. In other words, a large fraction of events add to
the Compton continuum rather than to the full energy peak, thus, making discrimination between neutrons
and background gamma rays difficult. However, with adequate energy resolution, pulse height discrimination
can be used to distinguish the prompt gamma-ray emissions from neutron interactions.
CdTe and CdZnTe have mass densities of 5.86 and about 5.8 g cm−3 and 2200-m/s macroscopic absorption
cross sections of 37.2 cm−1 and 34.8 cm−1 , respectively. Hence, over 95% of thermal neutrons are absorbed
within a 1-mm thickness of either material with most thermal neutrons being absorbed near the detector
surface. For detectors of typical thicknesses between 2 and 10 mm, nearly half of the gamma rays are
emitted in directions away from the detector bulk. This geometric problem, coupled with the low gamma-
ray attenuation coefficients for 558.6-keV and 651.3-keV gamma rays (see Fig. 16.1), mostly from Compton
scattering, yields a relatively low neutron detection efficiency. For instance, McGregor et al. [1996a] report
a thermal-neutron detection efficiency of only 3.7±1.9% for a 3-mm-thick CdZnTe detector, although the
device was capable of absorbing over 99% of the intersecting thermal neutrons. Using Cd starting material
Sec. 17.6. Neutron Diffraction 861

slightly depleted of 113 Cd tends to distribute neutron absorption more evenly throughout thick crystals;
however, this approach can be costly.
The problem of non-uniform neutron absorption is less pronounced for HgI2 , which has a density of 6.4 g
cm−3 and a 2200-m/s macroscopic cross section of 3.17 cm−1 . Because the neutron absorption is more evenly
distributed through the material, it takes approximately 1 cm of material to absorb 95% of thermal neutrons.
Further, the prompt gamma-ray emission energy of 368.1 keV has a higher linear attenuation coefficient, with
the photoelectric coefficient being slightly higher than the Compton scattering coefficient. Hence, the prompt
gamma rays resulting from 199 Hg(n,γ)200 Hg reactions have a higher probability of reabsorption compared
to that for the prompt gamma rays from CdTe and CdZnTe devices. Unfortunately, material problems with
HgI2 have not yet yielded results that support its widespread use for neutron detection. Further, because of
the high Z components, interference from background gamma rays becomes more of a problem so that good
energy resolution of the full energy peak is important.

17.6 Neutron Diffraction


The concept of wave-particle duality was introduced in Secs. 3.2.5 and 3.2.6, and Bragg diffraction was
briefly mentioned in Sec. 12.4. Described here is a method to use the wave nature of neutrons with Bragg
diffraction to measure the energy of slow neutrons. Recall from Sec. 3.2.6 that the de Broglie wavelength is
h h
λ= = . (17.39)
p mn v
where h is Planck’s constant, mn is the neutron rest mass, and v is the neutron speed. Given a neutron
energy, then Eq. (17.39) can be rewritten as

h
λ= √ . (17.40)
2mn E l
At low energies, relativistic effects can be ignored,
hence the rest mass of a neutron can be used to find
the de Broglie wavelength
q q
0.286
λn = √ Å (17.41) d q q
E
where λn is in angstroms and E is expressed in electron
volts (eV). d
The Bragg condition for diffraction is related to
wavelength by Figure 17.32. Geometry for Bragg diffraction of particles,
nλ = 2d sin θ, (17.42) showing the case for n = 4.

where n is an integer, d is the spacing between parallel atomic planes in an ordered crystal, and θ is the angle
at which radiation intersects the crystal from the direction parallel to the planes, as depicted in Fig. 17.32.
Elsasser [1936] predicted that neutrons could be diffracted from crystal planes, shortly thereafter proven by
experiments conducted by Halban and Preiswerk [1936] and Mitchell and Powers [1936]. Substitution of
Eq. (17.41) into Eq. (17.42) yields
0.286n
sin θ = √ , (17.43)
2d E
where d is in angstroms and E is in eV. Consider the fundamental diffraction condition with n = 1. Here it
is shown that given a distance d between crystal planes there is an lower limit to the neutron energy that
can be observed. Also, given a practical working angle θ, an upper energy limit can also be determined.
862 Slow Neutron Detectors Chapt. 17

Example 17.3: Given a lower diffraction angle limit of 1◦ , what are the neutron diffraction energy limits
for n = 1 of a Si crystal oriented for diffraction off the {111} planes.

Solution:
For silicon, a = 5.43 Å and the distances between planes are found from Eq. (12.4),

a 5.43 Å
d= √ = √ = 3.135 Å
h2 + k2 + l2 3
where (hkl) refer to the Miller indices of the crystal. The limits must lie between sin(1◦ ) and 1, hence
0.286
sin(1◦ ) ≤ √ ≤ 1.
2d E
Rearranging terms yields
6.83 eV ≥ E ≥ 0.00208 eV.

Although reflection and diffraction seem similar, in that the angle of incidence is equal to the angle
of emission, they are fundamentally different.
First, all atoms in the crystal along the path
of the incident beam participate in diffraction, transmission
whereas reflection is more or less a surface phe- method
nomenon (e.g., reflection of light). Diffraction
occurs only if the Bragg condition of Eq. (17.42) to
is met, while reflection can occur at practically
any angle. Reflection is a far more efficient pro-
reflection
cess than diffraction. For instance, practically
method
all photons are reflected from a specular sur-
face, whereas a diffracted beam comprises only
a few percent of the incident beam. Neutron Figure 17.33. Distinction between reflection and transmission cases
diffraction can be used in either reflection or of diffraction by a parallel crystal slab of thickness to . After Bacon
transmission modes [Bacon and Lowde 1948], [1975].
as depicted in Fig. 17.33. In either case, the ef-
fect of diffracted neutrons leaving the beam is bio-shield
called extinction. In other words, the strength moderator
of the neutron beam diminishes as neutrons are
diffracted out, thereby causing the diffracted collimator
beam to weaken as the diffraction depth in- w
q1 crystal
creases.
reactor a
The method of neutron diffraction can be
used to isolate specific energies of neutrons, q2
most effectively for slow neutrons. Such an ar- L r2
rangement is shown in Fig. 17.34. Consider the r1
detector
case in which moderated neutrons from a source
are collimated onto a perfect crystal. If the ori-
gin of the neutrons is considered a point cen- Figure 17.34. Common arrangement for a neutron diffractometer
tered at the collimator entrance, then neutrons at a nuclear reactor beamport. After Spalek [1965].
Sec. 17.6. Neutron Diffraction 863

may be diffracted at limits defined by rays r1 and r2 . Consequently, only those neutrons with wavelength
(energy) defined by θ1 in Eq. (17.42) diffract along ray r1 , while only those neutrons with wavelength (en-
ergy) defined by θ2 in Eq. (17.42) will diffract along ray r2 . Obviously, neutrons confined within these limits
will diffract only if the Bragg condition is also met. Hence, there is a spread of neutron wavelengths that
can diffract from the crystal with this configuration

n dλ = 2d cos θdθ. (17.44)

The angle α defined by the collimator is small, hence


w
dθ = α  (17.45)
L
where w and L are the collimator diameter and length, respectively. Note that neutrons may enter the colli-
mator at any location along the entrance orifice, which broadens the total spread in angle to 2α. Substitution
of these results into Eq. (17.44) yields
4wd
n dλ = cos θ. (17.46)
L
The resolving power η is a measure of the diffractometer ability to distinguish between neutron wavelengths,
generally defined as
λ L tan θ
η= = . (17.47)
dλ 2w
In reality, crystals have numerous imperfections in the structure. In fact, a so-called perfect crystal
without point defects will still have structural misorientations of crystal segments on the order of 500 nm
long, referred to as the crystal mosaic. The magnitude of the angular misorientation of these mosaic blocks,
called the mosaic spread, can range from a few minutes of arc up to a half a degree. Consequently, neutrons
can actually penetrate deeper into the crystal and diffract more efficiently over a range of mosaic angles.22
This increase in diffracted neutrons is generally proportional to the square of the crystal structure factor
(F 2hkl ) [Bacon 1966].

17.6.1 The Structure Factor for Crystals F hkl


The crystal structure factor F hkl is a mathematical method of describing the diffraction of waves in a
crystalline solid, which describes the amplitude and phase of the diffracted wave


N
Fhkl = bj e[2πi(hxj +kyj +lzj )] , (17.48)
j=1

where the sum is over all atoms (N ) in a unit cell, xj , yj , zj are the position coordinates of the jth atom,
and bj is the neutron scattering length of the jth atom. From Euler’s formula


N 
N
Fhkl = bj cos [2π (hxj + kyj + lzj )] + i bj sin [2π (hxj + kyj + lzj )] . (17.49)
j=1 j=1

The notation for the structure factor is often abbreviated as simply F .

22 Infact, diffraction crystals are purposely compressed under pressure to produce an optimum mosaic spread in order to increase
the strength of the diffracted neutron beam.
864 Slow Neutron Detectors Chapt. 17

Recall from Chapter 12 that the terms hkl refer to the Miller indices. Hence, the structure factor is the
result of all waves scattered in the [hkl] direction of reflection by the N atoms contained in the unit cell.
The structure factor for neutrons is described in terms of length with units on the order of 10−12 cm. When
considering a small volume of the crystal, dV , the total integrated diffraction under the reflection orientation
from this segment is
λ3 M 2 2
QdV = F , (17.50)
sin(2θB ) hkl
where M is the reciprocal of the unit cell volume, θB is the Bragg scattering angle, and λ is the de Broglie
neutron wavelength.
As neutrons proceed through a large crystal at the Bragg angle, the diffracted amplitude is reduced by
both neutron absorption and neutron diffraction. Thus, even after allowing for the effect of absorption, the
deeper parts of the crystal contribute less than the upper parts, because neutrons corresponding to the Bragg
condition of Eq. (17.42) are being removed before reaching lower crystal planes. Consequently, Eq. (17.50)
fails to describe the integrated diffraction for thick crystals, the phenomenon referred to earlier as extinction
[Bacon and Lowde 1948].

Example 17.4: Determine the structure factor of an FCC lattice.

Solution:
The unit cell has four complete atoms, with one located at the origin and three located at the adjacent
faces of the unit cubic cell. Hence, the coordinates for four adjacent atoms in the unit cell can be written as
 
1 1
x1 , y1 , z1 = (0, 0, 0); x2 , y2 , z2 = , ,0 ;
2 2
   
1 1 1 1
x 3 , y3 , z 3 = 0, , ; x 4 , y4 , z 4 = , 0,
2 2 2 2

For integer values of hkl and from Eq. (17.49) the structure factor becomes,

Fhkl = b (1 + cos[π(h + k)] + cos[π(k + l)] + cos[π(h + l)]) .

Consequently, if hkl are all even or are all odd, then Fhkl = 4b. However, if hkl is mixed odd and even, then
Fhkl = 0.

17.6.2 Angular Response to a Maxwellian Neutron Distribution


Consider the distribution of slow neutrons in a nuclear reactor, generally described by a Maxwellian distri-
bution
2 2
dn = K1 v 2 e−v /vo dv, (17.51)
where dn is the number of neutrons within differential speed dv about v per unit volume, and vo is the most
probable neutron velocity. The flux of neutrons of some speed v is simply the product v dn so intensity or
flux of neutrons traveling down the beam port is
2
/vo2
dnb = v dn = K1 v 3 e−v dv. (17.52)
Sec. 17.6. Neutron Diffraction 865

These neutrons strike the diffraction crystal, as depicted in Fig. 17.34. Neutron diffraction off the crystal
varies inversely with the neutron energy E or v 2 . Consequently, the diffracted beam (reflection condition)
spectrum from the neutron beam becomes
v dn 2 2
dnd = = K1 ve−v /vo dv. (17.53)
v2
According to Eq. (17.53), as the neutron velocity increases, the number of diffracted neutrons decreases
with v. Given any Bragg angle θB , the neutron velocities must satisfy Eq. (17.42) to undergo diffraction.
Neutrons that reach the neutron detector for select Bragg angles are of constant velocity. Hence, to map
a select neutron energy range, the crystal can be rotated in the neutron beam to change θB . The detector
position must also be changed by 2θB to match the Bragg angle.
From Eq. (17.39) and Eq. (17.44), one can derive
nh
− dv = 2d cos θ dθ. (17.54)
mv 2
Considering only the fundamental diffraction (n = 1), Eq. (17.54) can be rearranged to find

2mn v 2 d
dv = − cos θ dθ. (17.55)
h
Substitution of Eq. (17.55) into Eq. (17.53) yields

dnd 2mn v 3 d −v2 /vo2


= −K1 e cos θ. (17.56)
dθ h
The collimator geometry defines dθ and can be regarding as constant. Consequently, the detector response
C, or the count rate, is described by
2 2
C = K2 v 3 e−v /vo cos θ, (17.57)
and when divided by cos θ yields
C 2 2
= K2 v 3 e−v /v0 , (17.58)
cos θ
the same relative distribution as the slow neutron distribution in the beamport (Eq. (17.52)). Hence, this
outcome yields the thermal neutron flux in the nuclear reactor, while dividing by v yields the slow neutron
distribution in the nuclear reactor.

17.6.3 Measurements with Diffracted Neutron Beams


Diffracted neutron beams can be used to identify neutron energies provided that the Bragg condition under
use is well calibrated. Such uses apply to polyenergetic neutron sources, such as from a beamport from a
nuclear reactor. Another use of diffracted neutron beams is to study the crystallinity of crystals, where the
crystal under study is rotated through the beam about the Bragg angle. The resolution of the response
gives a measure of the crystal perfection, the response often referred to as a rocking curve. Another common
application is as a nearly pure monoenergetic neutron beam for measurements and experiments. Although
contamination may be present from higher orders of diffracted neutrons (n > 1) and scattered background
neutrons, the combined effects of Eq. (17.50) and Eq. (17.53) diminish this effect. This contamination can be
reduced further with a second diffraction crystal between the primary crystal and the detector. This second
crystal must be set at the same Bragg condition as the first crystal, which produces a somewhat stringent
alignment requirement between the two crystals, a tedious process, and comes with the expense of a lower
866 Slow Neutron Detectors Chapt. 17

overall neutron flux at the work location. From Eq. (17.47), the limiting energy resolution dE/E from the
beamport is,  
 dE  2dλ 4w
 
 E  = λ = L tan θ . (17.59)

With simple substitutions and use of trigonometric identities,


  √ 
 dE  4wd E cos θ 4wd E − (k 2 n2 /4d2 )
 
 E = nLk
=
nLk
, (17.60)

where d is the interplane distance and k = 0.286 from Eq. (17.43). If the Bragg angle is well known from the
crystal diffractometer, then the neutron energy is also known, and accurate measurements of neutron cross
sections can be performed for various intervening materials (between the crystal and detector), limited by
the energy resolution of the system.

17.7 Calibration of Slow Neutron Detectors


There are numerous methods used by credible organizations to calibrate and determine the neutron detection
efficiency of thermal neutron detectors. These methods can differ significantly with varying degrees of
measurement error. The reason for the differing calibration methods stems primarily from the difficulty
in securing a calibrated standardized neutron source. For thermal-neutron detection efficiency, a diffracted
neutron beam from a nuclear reactor is possibly the best calibration source. However, access to a nuclear
research reactor is often inconvenient, and an organization may instead resort to a moderated 252 Cf or AmBe
source. Fortunately, calibration of slow-neutron detectors can be a relatively straightforward process for 1/v
absorbers [McGregor and Shultis 2011]. A few of these calibration methods are described here, although they
do not represent the many methods used by various organizations. The different measurement protocols,
although reproducible, are often not easily related to each other.
According to National Institute of Standards and Technology (NIST), there is no reliable method to
produce an omnidirectional thermal neutron source to test a detector in an isotropic flux [McGregor and
Shultis 2011]. Monte Carlo codes such as MCNP can be used to understand the experimental conditions
and optimize a measurement, but it is inadequate to predict the detection efficiency, mainly because of the
uncertainty associated with the code (about 5%) and uncertainty with the neutron measurement (also about
5%) together produce a result that has an unacceptable error for NIST-traceable detector calibrations.

17.7.1 Method of the NIST


The NIST uses a combination of a calibrated neutron current and calibrated neutron detectors to determine
the unknown efficiency of a neutron detector [McGregor and Shultis 2011]. The calibration consists of using
a 252 Cf neutron source placed in a heavy-water moderator pool that approximates the thermal-neutron
environment inside a light-water reactor. However, the preferred method for testing a thermal-neutron
detector is with a single-crystal diffracted beam, whose spatial profile is determined from activation analysis
of a Dy foil, or is measured with a neutron-imaging detector so that the neutron beam profile is documented
within the workspace. The neutron flux is then measured with a calibrated fission chamber. Hence, the
basic method is to (1) profile the relative thermal-neutron beam intensity as a function of position and
then (2) measure the neutron current (or fluence) with a calibrated standard fission chamber. The count
rate of the unknown detector is then directly compared to the measured neutron current. Note that fission
chambers, typically fabricated with uranium as the neutron reactive material, deviate slightly from the ideal
1/v behavior. Hence, knowledge of the diffraction angle, and resulting neutron energy, is important for
making thermal corrections to the NIST calibration method.
Sec. 17.7. Calibration of Slow Neutron Detectors 867

17.7.2 Method of Reuter Stokes


A calibration method used by some commercial manufacturers of neutron detectors is to archive a so-called
“gold standard” for each neutron detector product. For instance, for one such manufacturer, a large box
formed by walls of 6-inch-thick high-density polyethylene (HDPE) is used as a moderator. The box has a
large open cavity in the center, and a neutron source (252 Cf) is inserted into the box, centered near one
of the walls. Gold activation foils (see next section) are then used to measure the thermal-neutron flux at
various locations in the box after the foil measurements are corrected for neutron self-absorption. In this
manner the neutron flux is mapped spatially inside the HDPE box. A detector is then placed inside the
box, at an angle, near a wall opposite that of the location of the 252 Cf source. A measurement is conducted,
correcting for spatial differences in the neutron flux. Afterwards, a NIST traceable detector is placed in the
box at the prior location of the test detector, and another identical measurement is conducted.
This measurement method yields relative efficiencies as compared to a NIST-traceable standard. Hence,
the method relies upon a fast neutron source moderated in a box that produces a thermal-neutron flux
incident on the detector from nearly 4π directions. Due to the nature of the source-detector configuration,
the neutron flux intersecting the detector is not uniform in direction or space. The Au foil calibration allows
approximate corrections for non-uniform distribution of thermal neutrons. This method is adequate for in-
house calibrations, but is not easily used for calibrations at other facilities. Finally, the method is probably
adequate for large neutron detectors, but has larger measurement uncertainty for small neutron detectors.

17.7.3 Method of ORNL


A method introduced at Oak Ridge National Laboratory (ORNL) also uses a 252 Cf source. The neutron
source is placed within a large block of HDPE capable of moderating and minimizing the leakage of neutrons.
A blind hole beamport is drilled into the HDPE block that is oriented towards the source, but still leaves
enough moderator between the drilled beamport hole and the 252 Cf to produce a thermalized neutron beam.
A borated shutter, composed of perpendicular jaws, is attached to the moderator block around the beamport
opening and is used to reduce the beam cross sectional area. The thermal-neutron flux at the testing location
is measured with a calibrated neutron detector. For additional verification, MCNP is used to calculate the
expected neutron flux and profile at the testing location and is quoted as having approximately 10% error
[McGregor and Shultis 2011]. The observed count rate, per unit area, from the detector being studied is
then divided by the measured thermal-neutron flux to determine the intrinsic neutron detection efficiency.

17.7.4 Method of Sampson and Vincent


The method of Sampson and Vincent, introduced primarily as a calibration system for 10 BF3 detectors, is
used to determine the efficiency for a narrow beam geometry of diffracted neutrons [Sampson and Vincent
1971]. Here the BF3 detector is placed end-on facing into the neutron beam from the diffractometer. The
monoenergetic neutron flux from the diffracted beam is calibrated by activation of a NIST-traceable Au foil.
The Au foil is placed between the detector and the emerging neutron beam. The beam is set at an arbitrary
diffraction angle θ from the monodirectional neutrons incident on the diffractometer. The energy and beam
angle are described by the Bragg diffraction condition

h
nλ = n √ = 2d sin θ, n = 1, 2, 3, . . . , (17.61)
2En mn
where λ is the neutron wavelength, d is the atomic interplane distance, mn is the neutron mass, h is Plank’s
constant, and En is the neutron kinetic energy. For a given direction θ, the diffracted beam has neutrons of
energy E1 (for n = 1) and also for neutrons of higher energy, the “harmonics” (n > 1).
868 Slow Neutron Detectors Chapt. 17

10
The gold foil is used to measure the neutron flux φ incident on the end of the BF3 detector. If the foil
is totally immersed in the beam, the saturation activity of the Au foil AAu
∞ is

AAu

φ= , (17.62)
Nd σaAu (E)
where Nd is the total number of Au atoms in the foil, and σaAu (E) is the Au microscopic absorption neutron
cross section at energy E. For negligible absorption in the foil, the detector count rate when exposed to the
beam is
R = in (E)φA, (17.63)
where A is the cross sectional area of the neutron beam incident on the detector and in (E) is the intrinsic
efficiency of the detector. Combine these last two equations to obtain
RNd σaAu (E)
in (E) = . (17.64)
AAu
∞ Sb

In this simplistic overview, the details of correcting the gold foil activity for self-absorption, fast neutron
flux components, and counter efficiency used to measure the foil activity have been omitted. Sources of
uncertainty with the Sampson and Vincent method include flux contamination from higher order diffraction
harmonics (mainly from the second-order contamination), uncertainty in the flux calibration due to a sizeable
neutron resonance in the Au foil at 4.9 eV, uncertainty in the measurement of the neutron beam area (Sb ),
and finally uncertainly in the dead region at the end of the detector that reduces the neutron flux before
encountering the high-field region of the detector. Sampson and Vincent report a correction for second order
effects, and also report a theoretical efficiency that takes into account the end window absorption effects and
neutron scattering.

17.7.5 Method of McGregor and Shultis


A method developed by McGregor and Shultis [2011] provides an in-house calibration standard and works
especially well for neutron detectors based on 1/v absorbers without introducing multiple sources of error.
This method requires a moderated neutron beam without contamination from fast neutrons. Isolation of
the thermal neutrons is accomplished by diffracting, from a graphite crystal, a neutron beam from a nuclear
reactor. The graphite crystal structure destructively interferes with diffraction of even harmonics, thereby
eliminating problems with the contamination from second harmonic diffraction. Two 1/v neutron detectors
are required for the calibration, along with a duplicate, but empty shell, of at least one of the two detectors.
The test detector to be used as the calibration standard is placed in the neutron beam, as shown in
Fig. 17.35(b), such that neutrons pass through the container walls and neutron reactive gas. A reference
detector is placed in the neutron beam beyond the calibration detector, also shown in Fig. 17.35(b). The
reference detector measures a count rate of

Rout = Rin e−Σw tw e−Σg tg exp−Σw tw = Rin e−2Σw tw e−Σg tg , (17.65)


where Rin is the neutron count rate from the reference detector before neutrons are attenuated by the test
detector and Rout is the neutron count rate measured by the reference detector after attenuation through the
test detector, Σw is the macroscopic cross section of the empty detector shell material, Σg is the macroscopic
cross section for the detection material (gas) in the test detector, tw is the shell material thickness, and tg is
the thickness of the neutron reactive material within the test detector. The transmission factor for the test
detector is
Rout
Td ≡ = e−2Σw tw e−Σg tg . (17.66)
Rin
Sec. 17.7. Calibration of Slow Neutron Detectors 869

reference
detector
(a)
neutron beam

reference
test detector detector
(b)
neutron beam

reference
empty detector shell detector
(c)
neutron beam

Figure 17.35. Method to produce a calibrated standard


detector. After the calibration, the test detector can be used
as a calibration standard for other 1/v neutron detectors. For
the method to function properly, the reference detector must
also be a 1/v detector [McGregor and Shultis 2011] .

Transmission through the empty shell detector is,


Rw
T2w = = e−2Σw tw , (17.67)
Rin
where Rw is the count rate from the beam attenuated by the empty detector shell. The transmission factor
for neutrons passing through the test detector 1/v absorber is,
Rout
Tg = = e−Σg tg . (17.68)
Rw
The fraction of the neutron beam attenuated by the absorber in the test detector reveals the fraction of
interactions in the test detector, but does not yield the detector intrinsic efficiency. The beam attenuated
by the neutron absorber was already attenuated by one wall of the detector shell. Hence, the fraction of the
neutron beam transmitted through one wall of the detector shell is,

Rw
T1w = = [e−2Σw tw ]1/2 . (17.69)
Rin
The intrinsic slow-neutron detection efficiency is,
σao −Σw tw
in = e (1 − e−Σg tg ), (17.70)
σto
870 Slow Neutron Detectors Chapt. 17

where σao is the absorption cross section leading to detectable events in the test detector and σto is the total
cross section at an arbitrary energy Eo . The total cross section σto is the total probability that a neutron
interacts with a target nuclei, including capture, fission, elastic scattering, and inelastic scattering. Because
inelastic and elastic scattering usually do not follow a 1/v dependence, the ratio of σao /σto deviates from
1/v behavior at moderately high neutron energies, and proper corrections must be made to account for the
differences. However, at low energies (generally below 10 eV), σao ≈ σto is a good approximation. Therefore,
substitution of Eq. (17.68) and Eq. (17.69) into Eq. (17.70) yields,
  
Rw Rout
in = 1− , (17.71)
Rin Rw
which is the intrinsic detection efficiency for the test detector. The test detector can be used thereafter as a
calibration standard, provided that the totality of the neutron beam intersects within the perimeter of the
detector active region.
From the discussion in Section 17.1, the count rates represented by Rin , Rout , and Rw are independent
of neutron energy for materials with 1/v cross sections. Because of the σao /σto ratio, corrections may apply
for 1/v absorbers if the neutrons in the beam have energies exceeding approximately 10 eV. Hence neutron
moderation is required for the measurements in order to avoid such corrections. Finally, if the detector under
test is composed of non-1/v absorbers for the neutron reactive material, such as, for example, 157 Gd, 113 Cd,
or 235 U, then it is necessary to apply the appropriate non-1/v corrections to the calculated efficiency, and
generally requires some knowledge of the neutron energies.

17.8 Neutron Detection by Foil Activation


In the early days before modern neutron detectors, measurement of a neutron field was often done by
irradiating small samples (usually in the form of foils) composed of elements (or isotopes) whose cross
sections varied differently with the incident neutron energy. The radionuclides produced in the sample by
neutron absorptions decay with the emission of radiation that can be measured. The rate at which radiation
is emitted by an irradiated sample after it was removed from the neutron field depended on the flux used to
irradiate the sample, the irradiation time, and the composition of the detecting material.
From the activity produced in the foils and the use of clever unfolding algorithms, the magnitude and
energy dependence of the neutron flux could be estimated. The foil activation method is also discussed in
Sec. 18.5.7 for fast neutron measurements. Although once widely used, the use of the foil activation method
is not as prevalent today as it once was, primarily as a result of better and newer neutron detectors. However,
one foil activation method is still in wide use and is the basis of several thermal neutron flux standards.
In this method a gold foil is activated and from its resulting activity, both the thermal and fast neutron
fluxes can be inferred. This one-foil method is widely accepted and, with appropriate correction factors, can
give excellent results.23 Other foils that have been used to measure the thermal neutron flux with the Cd
covered/bare foil technique described in this section are listed in Table 17.3.
If the flux φ(E) is constant throughout the volume Vd of a bare gold foil, then the rate of production Rb
of the radionuclide produced by the absorption of a neutron in gold is
 ∞  ∞
Rb = Nd σa (E)φ(E) dE = Vd Σa (E)φ(E) dE, (17.72)
0 0

where Nd is the number of gold atoms in the foil, σa (E) the microscopic absorption cross section of gold,
φ(E) the energy-dependent flux density, and E the neutron energy.

23 One could say, in more ways than one, this foil technique is the “gold standard” for measuring thermal neutrons.
Sec. 17.8. Neutron Detection by Foil Activation 871

Table 17.3. Some activation foils used for thermal neutron measurements. Only the most abun-
dant gamma rays are listed. Data are extracted mostly from ENDF/B [2017] and LM-KAPL
[2002].
Isotope Nat. 2200-m/s (n,γ) Trans. γ-rays (keV)
Element Half-Life
abundance cross section (b) isotope [yield%]

Ag 107 Ag 51.84 45 108 Ag 633.0 [1.76] 2.382 m


109 Ag 48.16 4.4 110m Ag 657.8 [95.61] 249.8 d
677.6 [10.70]
763.9 [22.60]
884.7 [75.0]
937/5 [35.0]
1384.3 [25.1]
1475.8 [4.08]
1505.0 [13.33]
1562.3 [1.22]
Au 197 Au 100 98.65 198 Au 411.8 [95.62] 2.694 d
Co 59 Co 100 16.9 60m Co 58.60 [2.060] 10.47 m
20.2 60 Co 1173.2 [99.85] 5.271 y
1332.5 [99.98]
Cu 63 Cu 69.17 4.503 64 Cu 345.8 [0.475] 12.70 h
65 Cu 30.83 2.169 66 Cu 1039.2 [9.23] 5.120 m
Dy 164 Dy 28.18 1700 165m Dy 515.5 [1.53] 1.257 m
0.5155 [0.015]
 950 165 Dy 94.7 [3.80] 2.334 h
In 113 In 4.29 56 114m In 190.3 [15/56] 49.51 d
558.4 [4.4]
725.2 [4.4]
2 114 In 1299.8 [0.139] 71.9 s
115 In 95.71 160 116m1 In 4.16.9 [27.2] 54.29 m
818.7 [12.13]
1097.3 [58.5]
1293.6 [84.8]
1507.6 [9.92]
1752.5 [2.36]
2112.3 [15.09]
42 116 In 1293.4 [1.30] 14.10 s
Mn 55 Mn 100 13.28 56 Mn 846.8 [98.85] 2.5789 h
1810.7 [26.9]
2113.1 [14.2]
872 Slow Neutron Detectors Chapt. 17

In Fig. 17.36 the thermal energy dependence of the neutron flux and of the total cross sections for gold
and cadmium is shown. Several features should be noted. Below the so-called thermal cutoff ET C  0.2 eV
the neutron flux has a Maxwellian distribution φM (E). As can be seen from the cadmium cross section, a
cadmium covered gold foil is activated primarily by neutrons with energies above the cadmium cutoff energy
ECC  0.4 eV. Further below ECC gold is seen to be almost a perfect “1/v” absorber.

Figure 17.36. The energy dependence of the thermal flux φM (E) for neu-
trons in thermal equilibrium at room temperature (T = 293 K), the idealized
epithermal 1/E slowing-down flux above the thermal cutoff ET C , and the total
(absorption) cross sections for gold and cadmium.

The total thermal flux density, or thermal flux for short, is defined as
 ET C
φt ≡ φ(E) dE, (17.73)
0

and the total fast flux as


 Emax
φf ≡ φ(E) dE, (17.74)
ET C
Sec. 17.8. Neutron Detection by Foil Activation 873

where Emax is the maximum neutron energy. Below the thermal cutoff ET C the energy distribution of the
flux can often be well approximated by the Maxwellian distribution (see Problem 17-1)
E −E/ET
φ(E)  φM (E, T ) = φt e , (17.75)
ET2

where ET ≡ kT (= 0.0253 eV for a neutron temperature of T = 293.5 K) is the most probable neutron
energy for the thermal flux density.
For E > ET C , the neutron flux in and from a reactor varies as 1/E or φ(E) = φo /E, characteristic of a
neutron slowing down spectrum. The total fast flux is thus
 Emax  Emax  
φo Emax
φf ≡ φ(E) dE = dE = φo ln . (17.76)
ET C ET C E ET C

For ET C  0.2 eV and Emax  20 MeV, φf  18φo . Below ET C gold is a 1/v absorber, i.e., σa (E) =
σa (Eo ) Eo /E where σa (Eo ) is the gold absorption cross section at an arbitrary thermal reference energy
usually taken as Eo = ET =293.5K = 0.0253 eV.
The activation rate for a bare gold foil may then be written as
$ √  Emax /
ET C
σa (Eo ) Eo φo
Rb = Nd √ φM (E, T ) dE + σa (E) dE (17.77)
0 E ET C E

or  Emax
φo
Rb = Nd σ a φt + Nd σa (E) dE (17.78)
ET C E
where the thermal-averaged absorption cross section for gold is
 ET C 
Eo
σa (Eo ) φM (E, T ) dE
E
σa ≡ 0  ET C 
φM (E, T ) dE
0
 ∞ 
Eo
σa (Eo ) φM (E, T ) dE √ 
E π To
0  ∞ = σa (Eo ). (17.79)
2 T
φM (E, T ) dE
0

If it is assumed φ(E) = φo /E for E > ET C then the integral in Eq. (17.78) can be evaluated as
 Emax  ECC   Emax
dE Eo 1 σa (E)
σa (E) = φo σa (Eo ) dE + φo dE
ET C E ET C E E ECC E

    Emax
1 1 σa (E)
= σa (Eo )φo 4Eo √ −√ + φo dE.
ET C ECC ECC E
    Emax
16ET 1 1 σa (E)
= σ a φo √ −√ + φo dE. (17.80)
π ET C ECC ECC E
874 Slow Neutron Detectors Chapt. 17

Substitution of this result into Eq. (17.78) gives the activation rate of a bare foil as

$     /
Emax
16ET 1 1 σa (E)
Rb = Nd σ a φt + φo σ a √ −√ + φo dE . (17.81)
π ET C ECC ECC E

To measure the thermal flux φt , one must differentiate between the activation produced by thermal
neutrons and by fast neutrons. One way to do this experimentally is to make two measurements, one with
a bare foil and one with a detector foil covered with cadmium of sufficient thickness to absorb all thermal
neutrons below the cadmium cutoff energy ECC from reaching the gold foil. However, neutrons with energies
above ECC reach the gold foil and activate it at a rate

 Emax
dE
Rc = Nd φo σa (E) ≡ Nd φo Id . (17.82)
ECC E

The integral in this expression is called the resonance integral Id of a detector foil element. Values of the
resonance integral for many elements have been measured and tabulated [ANL 5800]. For example, the
resonance integral for gold is 1558 b. From the rate of activation of the cadmium-covered foil, the value of
φo can be obtained. However, it must be recognized that the detector foil absorption cross section generally
has many resonances and there can be significant self-shielding in the foil at these resonance energies. Thus
the assumption that the flux is constant throughout the foil may be a poor assumption for the fast-neutron
activation of the foil. Correction for this and other non-ideal effects are considered later.
The difference between the activation rate of the bare and cadmium-covered foils is thus
$   /
16ET 1 1
Rb − Rc = Nd σa φt + φo √ −√ . (17.83)
π ET C ECC

For ET = 0.03 eV, ET C = 0.2 eV, and ECC = 0.4 eV, the coefficient of φo is about 0.25. The value of
φo is often sufficiently small that the second term on the right-hand side of Eq. (17.83) can be neglected.
However, one should, in principle, distinguish between the thermal flux contribution and the subcadmium flux
contribution from epithermal neutrons, even if, in practice, the thermal flux is assumed to be proportional
to Rb − Rc .

17.8.1 Cadmium Ratio


In flux measurements, one often encounters the term cadmium ratio (CR). This ratio is simply the specific
activation rates of bare and cadmium-covered foil detectors, i.e.,
>b
R
CR ≡ (17.84)
>c
R
where the specific activation rate R ≡ R/m with the foil mass denoted by m. From the results of Eqs. (17.81)
and (17.82), the CR is
$   /
σ a φt 16ET 1 1 φt σ a
CR = 1 + + √ −√ 1+ . (17.85)
Id φo π ET C ECC φo Id
Sec. 17.8. Neutron Detection by Foil Activation 875

where the last simplification is obtained by ignoring the usually very small subcadmium epithermal activation.
From this result, it is evident that the larger the measured value of the CR, the larger is the proportion of
thermal neutrons in the total neutron population reaching the detecting foils.

17.8.2 Measuring Activation Rates


Thus far, only the rates of production of radioactive foil atoms have been considered. In this section
production rates are related to measurable quantities. After irradiation, it is the activity of the foil that is
actually measured, which usually persists some time after the irradiation procedure. Thus it is necessary to
relate the foil activity A to the production rate R of radionuclides in the foil during the irradiation process.

Figure 17.37. Activity of a foil that is irradiated by a constant flux between times 0
and t1 . At time t1 the foil is removed from the neutron beam. The foil is subsequently
counted between times t2 and t3 .

The buildup of radionuclides in a foil during irradiation is described by


dN (t)
= R − λN (t), (17.86)
dt
where N (t) is the number of radionuclides (with decay constant λ) in the foil at time t after the commence-
ment of irradiation. Burnup of the parent and daughter nuclides can usually be neglected. If the foil was
“clean” at the time (t = 0) irradiation began, then the number of radionuclide daughters at a later time t is
R: ;
N (t) = 1 − e−λt , (17.87)
λ
and the foil activity at time t is : ;
A(t) ≡ λN (t) = R 1 − e−λt . (17.88)
If the foil remains in the neutron flux for a time much greater than the half-life of the daughter radionuclide,
the activity reaches its saturation value A∞ = R, the sought quantity. After removal of the foil at time t1 ,
the activity exponentially decreases as
: ;
A(t) = A(t1 )e−λ(t−t1 ) = R 1 − e−λt1 e−λ(t−t1 ) , t > t1 . (17.89)

By counting the radiation emitted by the radioactive foil we can determine R. Suppose, the radionuclide
emits a gamma ray of energy E0 with a frequency f per decay. A gamma-ray spectrometer with known
876 Slow Neutron Detectors Chapt. 17

efficiency (E0 ) at gamma-ray energy E0 is used to measure the activity of E0 emitted from the foil between
times t2 and t3 (from Fig. 17.37). The total observed counts in the photopeak is
 t3  t3
C = f A(t) dt + BG = f  A(t1 )e−λ(t−t1 ) dt + BG
t2 t2

f A(t1 )eλt1 : −λt2 ;


= e − e−λt3 + BG
λ
f R : λt1 ;: ;
= e − 1 e−λt2 − e−λt3 + BG (17.90)
λ
where BG is the background count that occurred between t2 and t3 . From this result the production rate R
(equal to the saturation activity A∞ ) is found to be

λ(C − BG)
R = A∞ = . (17.91)
f (eλt1 − 1)(e−λt2 − e−λt3 )

To obtain R from the above expression, it is necessary to first obtain the counter efficiency  for the counting
geometry and radiation emitted by the foil’s radionuclides.
Foils used in a neutron flux measurement usually have different masses. To correct for the different
masses, the specific foil activity is calculated, i.e., the activity per unit mass of the foil. From Eq. (17.91)
the specific activity is
≡ R = λ(C − BG)
R . (17.92)
m mf (eλt1 − 1)(e−λt2 − e−λt3 )
Finally, the confidence limits on the variance of R  are obtained from the variances of the foil and background
counts, and the uncertainties in the times t1 , t2 , and t3 .
Natural gold consists of only the stable 197 Au isotope. Upon absorption of neutrons, radioactive 198 Au
is produced. This isotope has a half-life of 2.696 d and decays by β − emission. In the decay process a
0.4118-MeV gamma ray is emitted with a frequency of 95.51%. Other emitted gamma and x-ray photons
have frequencies of less than 2%. Activity measurements of the gold foils are performed with a gamma-ray
spectrometer (usually a high-resolution HPGe detector) by measuring the counts in the 411-keV full energy
peak. The absolute spectrometer efficiency  at this energy and the sample position must be obtained by
using calibration sources.

17.8.3 Flux Correction Factors


The theory presented so far has neglected some minor effects which require corrections to obtain accurate
flux values. Specifically, the following facts have been neglected:
1. Gold is not exactly a 1/v absorber at the high end of the Maxwellian spectrum (see Fig. 17.36).
2. Some neutrons with E < ECC pass through the cadmium cover and activate the covered gold foil.
3. The cadmium cover also stops some neutrons with E > ECC , so fewer fast neutrons activate a covered
gold foil compared to a bare foil.

4. If the detector foils are measuring the flux in a medium through which neutrons are diffusing, the
presence of the foil with its relatively high absorption cross section causes the flux around the foil to
be depressed. For neutrons streaming through a void or in air, no such flux depression occurs.
Sec. 17.8. Neutron Detection by Foil Activation 877

5. At neutron energies for which the gold foil has a large cross section, the outer layer of the foil shields
the inner foil volume, i.e., the activation per unit volume is not uniform throughout the foil. This is
particularly important for the fast neutron activation of gold foils.
A detailed discussion of these complicating factors is beyond the scope of this book. Here only a brief
description of how these effects can be investigated is presented. Greater detail for the theory and methods
used to correct experimental data for these complicating factors are given in the references.

17.8.4 Correction for Non-1/v Absorption


To account for the first effect, a corrected thermal averaged cross section is used. The thermal averaged
cross section of Eq. (17.79) is more correctly defined as
 ∞
σa (E)φM (E, T ) dE √ 
0  π To
σa ≡ ∞ = ga (T ) σa (Eo ), (17.93)
2 T
φM (E, T ) dE
0

where ga (T ) is the Westcott non-1/v correction factor (see Eq. (17.13)) obtained by evaluating the above
integrals numerically. For a perfect 1/v absorber ga = 1, and for a gold foil in a Maxwellian neutron energy
distribution at room temperature (T = 293 K), ga (293 K) = 1.005 [ANL 5800]. However, as the neutron
temperature T increases the Maxwellian “hardens” as it shifts towards the gold absorption resonance at
E = 4.90 eV (see Fig. 17.36) and ga (T ) increases as gold becomes more non-1/v. However, near room
temperature one can set ga (T )  1 for gold without introducing significant error.24

17.8.5 Correction for Cadmium Filter Effects


Ideally, a high-pass neutron filter would absorb all neutrons below a sharp cutoff energy and be transparent
to neutrons with energies above the cutoff. A cadmium cover with a thickness of between 0.5 to 1 mm comes
close to this ideal, absorbing almost all neutrons below about 0.4 eV and only a few above about 0.6 eV.

Figure 17.38. Foil saturation activity for dif- Figure 17.39. Epithermal cadmium correc-
ferent thicknesses of cadmium covering the foil. tion factor FCd for covers of different thick-
nesses.

The effect of a cadmium filter covering a gold foil can be investigated by irradiating detector foils with
different thicknesses of the cadmium cover. A typical plot of such results is shown in Fig. 17.38. The actual

24 Data
for ga (T ) and the resonance integral needed for other foils used in activation analyses can be found in ANL [2003],
Mughabghab [2003], and on-line at wwwnde.jaea.go.jp/j40/j40.htm.
878 Slow Neutron Detectors Chapt. 17

shape of the curve depends on several factors such as the detector foil material, foil size, the medium in which
the measurements are made, and the cadmium ratio. From Fig. 17.38, the rapid rise below approximately
20 mil (∼ 500 microns) of cadmium indicates that a significant number of subcadmium neutrons reach the
foil. More than 20 mils (∼ 500 microns) of cadmium seems to reduce the subcadmium transmission enough
so that the curve has only a small slope (caused by the cadmium absorption of epi-cadmium neutrons). For
cadmium thicknesses greater than about 20 mils, one can correct for the absorption of epi-cadmium neutrons
by extrapolating to zero cadmium thickness (the straight line in Fig. 17.38).
If a cadmium cover of thickness 500 microns or more is used, negligible thermal neutrons reach the gold
foil. However, this cover absorbs some epithermal neutrons. To correct for this, a cadmium filter correction
factor FCd is defined as
Repi
FCd ≡ , (17.94)
Rc
where Repi is activation rate in a bare foil by epithermal (above thermal) neutrons and Rc is the measured
activation rate in a cadmium covered foil by epithermal neutrons. For a gold foil most of the epithermal
activation is caused by neutrons absorbed in the gold resonance at Er = 4.91 eV. If α represents the
probability a 4.91-eV neutron passes through a cadmium cover of thickness tc

Repi Repi 1
FCd ≡ = = . (17.95)
Rc αRepi α

For a beam of 4.91-eV neutrons normally incident on the cadmium cover, α = exp[−ΣCd (Er )tc ] ≡ exp[−τc ].
Then for a normally incident beam of neutrons

FCd = exp[τc ]. (17.96)

For a covered foil placed in an isotropic flux, it can be shown [Profio 1976], α = 2E3 (τc ) so that

1
FCd = , (17.97)
2E3 (τc )

where E3 (x) is the exponential integral function of order 3. These factors for a gold foil are shown in
Fig. 17.39. Thus, to correct for epithermal-neutron absorption in the cadmium covered foil, we should use
Repi = FCd Rc in place of Rc in Eqs. (17.81) to (17.83) which are used to calculate the fast and thermal flux
densities.

17.8.6 Correction for Flux Perturbation and Self-Shielding


The complicating effects of foil self-shielding and the depression of the neutron field around the foil can be
investigated by irradiating foils with the same area but different thicknesses. A typical result is shown in
Fig. 17.40. The shape of such a plot depends on the area of the foil, the foil material, and the medium
in which the measurements are made. The effect of flux depression and self-shielding can be eliminated
by extrapolating the experimental results to zero foil thickness. Previous investigators have analyzed these
complicating factors both analytically and experimentally, and several semiempirical correction factors have
been developed [ANL 5800].
When an absorbing foil is used to measure the flux (fast or thermal) at some point in a moderator, the
foil causes a depression in the flux around the foil. Moreover, the flux is depressed in the center of the foil
because of self-shielding. A typical flux-profile is shown in Fig. 17.41. The average flux φ is found through
the through measuring the foil activity. However, it is the unperturbed flux φ∞ that is sought. These two
Sec. 17.8. Neutron Detection by Foil Activation 879

absorbing foil

fs
f

Figure 17.40. Saturation activity per unit vol- Figure 17.41. The depression of the flux and
ume for different thicknesses of foil. the self-shielding effect produced by an absorbing
foil in a moderator.

flux densities are related by


  
φ φs 1
φ= φ∞ or φ∞ = φ, (17.98)
φs φ∞ F1 F2

where the self-shielding factor F1 ≡ (φ/φs ) and the flux-depression factor F2 ≡ (φs /φ∞ ). In general, these
correction factors depend on the angular distribution of the flux density, foil size and thickness, and on
the scattering and absorption cross sections of the surrounding material. Two extreme cases of angular
distribution of the flux are considered below.
Perpendicular Beam in Air
In this geometry, the foil is placed in a non-diffusing medium and irradiated by a perpendicular beam of
neutrons. The flux of the beam is not affected by the foil so that F2 = 1 and φs = φ∞ .
Thermal Flux-Density Self-Shielding: For a foil with Σa Σs whose radius is much greater than its
thickness d, and which is irradiated by a perpendicular beam of thermal neutrons with a Maxwellian energy
distribution, the position dependent neutron flux is,

φ(x) = φs e−Σa x , (17.99)

where x is distance into the foil. For a thin foil, there


√ is negligible spectrum hardening of the Maxwellian as
the neutrons pass through the foil so that Σa = ( π/2)Σao . Then the average flux in the foil to the incident
flux is     
φ φ 1 d −Σa x 1
F1 ≡ = = e dx = [1 − e−τ ], (17.100)
φs φ∞ d 0 τ
where τ ≡ Σa d.
Epithermal Flux-Density Self-Shielding: In the epithermal region, the absorption cross section is divided
into two portions (see Eq. (17.80)): a 1/v component between the thermal and cadmium cutoff energies, and
the component above ECC whose absorption is dominated by absorption resonances. The self-shielding in the
1/v region is negligible compared to that in the resonance region. In gold most of the fast absorption occurs
max
in the large resonance at 4.91 eV with a peak value of σar  30, 600 b. In the case of an isolated resonance
880 Slow Neutron Detectors Chapt. 17

without significant Doppler broadening, the fast self-shielding factor for a thin foil without appreciable
scattering can be approximated by [Profio 1976]

F1 = e−τr /2 [I0 (τr /2) + I1 (τr /2)], (17.101)

where τr is the thickness of the foil in mean-free-path lengths evaluated at the peak resonance energy, i.e.,
max
τr = Nd σar d, and I0 and I1 are the modified Bessel functions of the first kind of the zeroth and first order,
respectively.
Nearly Isotropic Flux Density
In this geometry, the foil is placed in a diffusing medium where the neutron field has an angular distribution
that is well described by just the P0 and P1 Legendre components, i.e., is nearly an isotropic field. In such
a field the volume averaged neutron absorption in the foil is nearly independent of the foil orientation.
Thermal Flux-Density Self-Shielding: The self-shielding correction factor for a nearly isotropic thermal
flux is given by [ANL 5800]
1 1
F1 = − E3 (τ ) , (17.102)
τ 2
where E3 is the exponential integral function of order three.
Resonance Self-Shielding: For isotropic neutron incidence on the foil, the self-shielding correction factor
for resonances is [Profio 1976] 
τr ∞ 2 −y
F1 = y e [I0 (y) + I1 (y)] dy. (17.103)
2 τr /2
Other expressions for F1 are [ANL 5800]

4 1
F1 = √ √ “thick foils” (17.104)
3 π τr

and
τr ln τr
F1 = 1 + − 0.3274τr “thin foils”. (17.105)
4
Thermal-Neutron Flux-Density Depression: The thermal-neutron flux can be severely depressed in the
vicinity of a strong absorber and thermal neutrons absorbed in the foil can no longer pass through the foil
and subsequently be reflected back to the foil and increase the foil activity. By contrast, fast neutrons passing
through a foil at resonance energies are degraded below the resonance energies in the moderator before they
are reflected back to the foil. Thus, for fast neutrons, the flux depression factor correction is close to unity,
i.e., F2fast = 1.
For thermal neutrons, the flux-depression correction factor can be expressed as [ANL 5800]
" #−1
1
F2th = 1+ − E3 (τ ) g(R, γ) , (17.106)
2

where γ ≡ Σs /Σt  1 for the moderator. Several expressions for the g-factor have been derived [ANL 5800].
One expression for g(R, γ) is [Profio 1976]
"       #
3 L 2R 2R
g(R, γ) = S −K ,γ rg . (17.107)
2 λ L L
Sec. 17.9. Self-Powered Neutron Detectors 881

Collector
(a)
Signal Wire Epoxy Seal
(Inconel)

Sensor Insulator Emitter Insulator Coaxial Sheath


(Al2O3) (MgO) (Inconel)

g (7) g (3) n
(6) n (4)
- -
(b)
- e -
b e b b
-

g
-
- e- e- b
e

(2) n n (5)
(1) n g (8) g (9)

Figure 17.42. (a) The basic components of an SPND; (b) Various radiation
interactions that can occur in an SPND.

Here S is the Skyrme function, 


4 1 
S(x) = 1 − e−xt 1 − t2 dt, (17.108)
x 0
K is a small transport correction that can be approximated by


⎨ 1 2R 2R ≤ λs
K 15 λs , (17.109)

⎩ 0.15 2R > λs

and rg is a factor depending on L/λ and varies between 0 and 0.9 [Ritchie and Eldridge 1960]. The moderator
parameters L, λ, and λs are the diffusion length, total mean-free-path length, and the scattering mean-free-
path length for thermal neutrons, respectively, in the moderator.

17.9 Self-Powered Neutron Detectors


The self-powered neutron detector (SPND) was originally introduced by J.W. Hilborn [1964].25 The name
“self-powered” is appropriate because these detectors operate without the need for an applied bias. Indeed,
they provide a current that is proportional to the neutron absorption rate, a current that can be easily
read with a femtoammeter. They are designed as in-core instrumentation for nuclear reactors, usually for
operation under steady-state conditions. SPNDs operate on the same principle as neutron activation analysis,
except the radioactive decay is rapid and the resulting activation is recorded in real time.
The construction of a basic SPND is shown in Fig. 17.42(a). The components include a neutron absorbing
emitter, an electrically conductive collector, and an insulating medium between them. Because these detec-
tors are inserted directly into the core of a nuclear reactor, the materials of choice must be radiation hard in
order to survive the total radiation fluence over their operating lifetime. The insulator is typically composed
of either aluminum oxide or magnesium oxide, both of which have relatively small neutron interaction cross

25 In some older texts and publications, they are referred to as Hilborn detectors.
882 Slow Neutron Detectors Chapt. 17

Figure 17.43. Radiative capture cross sections for 103 Rh, 51 V, and 59 Co.

Data are from [ENDFPLOT, 2015].

sections. Both insulators have high resistivity at room temperature and at the usual operating temperature
of a nuclear reactor core, where the resistivity varies from 1012 Ω-cm at room temperature to 5 × 108 Ω-cm
at 300 ◦ C. The resistivity of the insulating material will change over time with radiation damage, yet these
changes are comparable for both Al2 O3 and MgO for high purity materials [Angelone et al. 2014]. The
neutron cross section is lower for MgO than Al2 O3 and is typically used for the signal cable insulator. Both
Al2 O3 and MgO are used for the emitter insulator [Stevens 1973].
The conductive metal sheath is usually fabricated from Inconel, a relatively oxidation and corrosion
resistant austenite metal alloy of Ni, Cr, and Fe. Different Inconel alloys may include other elements to
improve specific properties. Inconel 600 is a common collector choice because of its resistance to corrosion
by high purity water, excellent oxidation resistance, high tensile strength, and resistance to stress cracking
at high temperatures. The emitter is a neutron activation material that produces daughter products with
relatively short decay times. These emitter materials must have thermal-neutron (n,γ) cross sections large
enough to be useful for activation, yet small enough so that burnup does not cause large changes in the
activation rate over time. The emitter sensitivity should be selective for neutrons or gamma rays. Further,
the preferred decay products are beta particles or conversion electrons, although gamma-ray emissions can be
used. Typical choices include rhodium, vanadium, and cobalt as emitter materials (whose cross sections are
shown in Fig. 17.43), although several other candidate materials have been studied [Hilborn 1964; Ramı́rez
and David 1970; Goldstein and Todt 1979; Amu and Petitcolas 1989; Imel and Hart 1996]. SPNDs are
available with short emitter active lengths of only 3 to 4 cm up to long active lengths greater than 20 cm.
For activated beta particle emitters, such as 103 Rh and 51 V, the emission of beta particles from the
emitter creates an electron current, i.e., the electrons that leave the emitter induce charge to flow through the
emitter lead and thus produce a current that can be monitored by a femtoammeter. For activated gamma-
ray emitters, the gamma rays can interact in the emitter and produce energetic electrons (photoelectric,
Compton), which also leave the emitter and produce an induced current. These beta particles, which are
Sec. 17.9. Self-Powered Neutron Detectors 883

electrons, may strike the collector; however, it is not necessary that these particles reach the collector to
produce a current. The mere action of the electrons leaving the emitter produces the induced current.
Recall from Sec. 8.5 that mobile charge moving between electrodes induces an image charge to appear on the
electrodes. Throughout much of this text, charges were influenced into motion by an electric field. However,
in the case of an SPND the electron velocity is produced by the kinetic energy imparted through the decay
process. Because beta particles are emitted as a continuous spectrum, with each decay sharing energy with
the recoil nucleus and an antineutrino, some beta particles have nearly zero energy while others retain the
maximum allowable energy. Consequently, some beta particles will not emerge from the emitter. Regardless,
the amount of current produced is a function of the emitter activity and, hence, the measured current is a
function of the neutron interaction rate in the emitter.
An analysis on the operation of SPNDs by Warren and Shah [1974] takes into consideration the influence
of space charge. Electrons do not freely conduct across the insulator between the emitter and collector.
Consequently electrons that come to rest in the insulator build up space charge over time, which ultimately
can produce an electric field. Already proven in Sec. 8.6.1 is the fact that space charge does not change
the induced current of an electron as it passes through a medium. However, the negative space charge can
work to produce a repulsive force that slows down the beta particle. Warren and Shah [1974] calculate that
a toroidal electric field maxima will appear in the insulator at some distance (dρ − dl )/2 from the emitter
surface, where dl and dp are the diameter of the emitter and the electric field maxima, respectively. Hence,
the amount of current induced by the beta particles and electrons can be reduced if the linear pathlength
is reduced. Also, electrons that are coulombically repelled backwards will produce a net induced current
representative of the net distance traveled between the emitter and collector. Electrons repelled back to the
emitter surface will, consequently, produce a net induced current of zero. A similar situation can be expected
for electrons emerging from the collector into the insulator.
Given a thermal-neutron, free-field, flux φ∞ , the average thermal flux φ in the emitter is given by
Eq. (17.98) or φ = F1 F2 φ∞ . For this simplistic analysis, the nuances of thermal neutron absorption and non
1/v cross section behavior discussed in Section 17.1 are ignored. The rate, per unit volume, of production
of the radioactive transmutation product from the emitter material is given by

R1 (t) = Ne σe φ exp[−σe φt], (17.110)

where Ne is the atomic density of emitter atoms and σe is the microscopic activation cross section of the
emitter material. Here it is assumed there is negligible burnup of the emitter atoms, i.e., Ne remains constant.
The atomic density N1 (t) of the radioactive transmutation product accounting for both radioactive decay
and transmutation is described by

dN1 (t)
= R1 (t) − σ1 φN1 (t) − λ1 N1 (t), (17.111)
dt
where σ1 is the thermal absorption cross section of the radioactive transmutation product and λ1 is its
radioactive decay constant.
Substitution of Eq. (17.110) into Eq. (17.111) and use of the initial condition N1 (0) = 0 yields the
following result for the activity of the daughter

λ1 Ne σe φ : ;
λ1 N1 (t) = exp[−σe φt] − exp[−(λ1 + φσ1 )t] . (17.112)
λ1 + (σ1 − σe )φ

The amount of current produced is also a function of the escape probability of beta particles and electrons
from the emitter. A correction constant K is often used to account for this escape probability, which is
884 Slow Neutron Detectors Chapt. 17

an intrinsic function of the emitter geometry and the beta particle emission spectrum. The current is then
determined by multiplying the above activity by the emitter volume Ve and by the unit charge constant, i.e.,
qn̄KVe λ1 Ne σe φ : ;
I(t) = exp[−σe φt] − exp[−(λ1 + σ1 φ)t] , (17.113)
λ1 + (σ1 − σe )φ
where n̄ is the average number of radiation quanta emitted per decay of N1 . Typically the emitter material
is relatively thin, on the order of 0.5–2 mm in diameter so as to reduce the neutron self-shielding. If emitters
with low absorption cross sections for both the initial and transmuted materials are used, then both the
neutron self-shielding and flux depression are negligible. Hence, Eq. (17.113) reduces to
: ;
I(t)  qn̄KVe Ne σe φ∞ 1 − e−λ1 t . (17.114)
The time response of an SPND is strongly dependent upon λ1 , with a large λ1 producing a rapid response
and a small λ1 yielding a delayed response. Properties of several emitters are listed in Table 17.4. As t
increases to relatively long operating times (t → ∞), the saturation current is reached and Eq. (17.114)
becomes
Isat (t)  qn̄KVe Ne σe φ∞ . (17.115)
For practical applications, 0.984Isat is reached at six half lives of the activated material. Hence, after a
step change in nuclear power, it takes 4 min 14 sec for a Rh emitter and 22 min and 36 sec for a vanadium
emitter to reach 98.4% of the new steady-state condition.
Shown in Fig. 17.42(b) are several possible reactions that can occur in an SPND [Moreira and Lescano
2013]. Events (1) through (5) are from neutron captures and events (6) through (9) are from direct gamma-
ray interactions. For events (1), (2), and (6), the loss of an electron or beta particle from the emitter causes
a net positive charge on the emitter, which causes electrons to flow towards the emitter from the signal cable,
thereby producing a positive current on the electrometer. For events (5) and (7), the loss of electrons or beta
particles from the collector produces a net positive charge on the collector, which causes negative current to
flow in the circuit. Events (3) and (8) add negative charge to the collector, which causes positive current to
flow in the signal cable, while events (4) and (9) produce negative charge in the emitter and cause negative
current flow in the signal cable. Ultimately, all of these events are possible, and the overall measured signal
is the net induced current response. If the emitter is designed such that most neutron interactions occur
in it while reducing gamma-ray interactions in the surrounding insulator and collector, then most of the
measured signal is from neutron absorptions in the emitter, and the neutron flux can be determined from
Eq. (17.115).
Neutron activation and gamma-ray interactions in the signal cable may cause background current, which
would overestimate the actual neutron flux at the emitter. To remedy this situation, many SPNDs are
available with twin leads in which both extend the distance of the entire cable, but only one is connected
to the emitter. The second lead produces a compensating signal, which can be subtracted from the primary
emitter lead signal in a similar fashion as in a compensated ion chamber.
Rhodium SPNDs are the most popular version in commercial use, mainly because of their higher sensitiv-
ity to neutrons than other emitter materials (see Table 17.4). Increased sensitivity, consequently, also means
higher burnup at a rate of ≈ 3.5% per month in a thermal-neutron flux of 1014 cm−2 s−1 . Rhodium emitters
have a relatively short half-life of 42.3 seconds for approximately 92.4% of the emissions, but also have a
longer delayed component for the remaining 7.6% of emissions. These delayed emissions are a consequence
of neutron captures producing an excited state of 104m Rh with a decay to ground state half-life of 261.6
seconds [Lederer and Shirley 1978].26 After this decay to ground, the 104 Rh decays by beta emission, with

26 This
half-life of 4.4 minutes is sometimes incorrectly presented as beta emission decay, which it is not. It is the half-life of the
metastable state 104m Rh to decay to the ground state of 104 Rh, which then subsequently decays by beta particle emission
Sec. 17.9. Self-Powered Neutron Detectors 885

Table 17.4. Properties of several SPND emitter materials with 508-μm diameters. The type of
reaction refers to how current is induced in the emitter, i.e., [n,β − ] indicates the daughter nuclide
undergoes beta decay and [n,γ] indicates capture gamma rays produce recoil electrons from scatters
in the SPND. The monthly burnup is for the SPND exposed to a flux of 1014 cm−2 s−1 . Data are
from Hilborn [1964]; Böck [1976]; Goldstein and Todt [1979].

Isotopic 2200-m/s daughter max Eβ Sensitivity Mon. %


Nuclide Reaction
Abund. σ (b) T1/2 (s) (MeV) (A s/cm3 ) burnup
103 Rh 100% 134 → 104 Rh 42.3 [n, β − ] 2.44 1.2 × 10−21 3.9
103 Rh 100% 11 → 104m Rh 261.6 none
51 V 99.75% 4.92 226 [n,β − ] 2.47 7.7 × 10−23 0.12
59 Co 100% 37.2 prompt [n,γ] 1.7 × 10−23 1.0
Nat. Pt 10 prompt [n,γ] 1.3 × 10−22 0.25
195 Pt 33.83% 27.5 prompt [n,γ]
107 Ag 51.35% 27.6 143 [n,β − ] 1.56 0.9
109 Ag 48.65% 90.3 24.6 [n,β − ] 2.87 2.3
27 Al 100% 0.233 135 [n,β − ] 2.87 0.006

T1/2 = 42 seconds, to stable 104 Pd. The expected activity, and therefore current, is depicted in Fig. 17.44
for a step increase in reactor power at t = 0 and a subsequent step decrease to zero power at t = 30 min.
Prompt increases in reactor power cannot be monitored with Rh-SPNDs because of these delayed signals.
Further, a step decrease in reactor power as shown in Fig. 17.44 serves to illustrate the issue; however this
scenario is somewhat artificial because reactor power cannot be reduced in a step-like manner but decreases
at its fastest with an 80 s period because of delayed neutrons. In short, Rh-SPNDs, like most SPNDs, are
good for steady-state power monitoring, but not for measuring power transients.
Vanadium SPNDs are also commercially available. With a half-life of 226 seconds, V-SPNDs have a
slower response than Rh-SPNDs. V-SPNDs are also less sensitive to neutrons and produce a much lower
output current. Although the lower sensitivity produces lower signal strengths, it serves to reduce burnup
and extend the SPND life to over 30 times that of a Rh emitter of the same size. For longevity, V-based
SPNDs have become popular in power reactors, mainly because they can be operated over a long period of
time with minimal burnup. As with Rh-SPNDs, V-SPNDs are good for steady-state power measurements,
but are not useful for monitoring power transients.
Emitters fashioned from Co perform as prompt flux monitoring devices. The prompt reaction
59
Co(n,γ)60 Co produces energetic gamma rays between 58 keV and 7.49 MeV, with predominant emissions
at 230 keV, 277 keV, 447 keV, 556 keV [see Lone et al. 1981; Tuli 1997]. The activation gamma rays can
be reabsorbed or scattered in the emitter material, both processes producing energetic electrons, although
these reabsorptions are relatively inefficient (1–2%) in such a small device [Goldstein and Todt 1979]. If the
electron exits the emitter, the net positive condition of the emitter causes charge to flow in the signal wire,
thereby producing current. The main advantage of Co-SPNDs is the prompt response that allows them to
follow better reactor transients and step changes in power.
However, the gamma rays can also interact in the sheath material and the insulator material. If energetic
electrons exit the sheath from gamma-ray interactions, then the result opposes the desired emitter emissions.
The same is true if a Compton or photo-electron enters the emitter from reactions in the insulator. Another
problem with SPNDs that rely upon (n,γ) reactions is the large gamma-ray background of a nuclear reactor.

with a half life of 42 seconds. The two half lives are not additive. The beta particle activity is determined by simultaneously
solving the differential equations of the decay scheme.
886 Slow Neutron Detectors Chapt. 17

Figure 17.44. Percent ratio of activity from 104 Rh and 104m Rh to that of
the activity of 104 Rh at steady-state equilibrium. The left side of the graph
depicts the increase to saturation for an immediate step increase in power from
zero, and the right side of the graph depicts the activity for an immediate step
decrease to zero. See text for details regarding issues with this simple model.

These background gamma rays can also interact in the emitter, insulator, or collector, adding either to the
emitter or collector currents. Hence, Co-SPNDs are designed such that the net current signal is produced
from emitter absorptions, which may be only 10–20% of the total interaction rate [Goldstein and Todt 1979].
Consequently, the inefficiency of capturing the prompt gamma-rays along with the competing interaction
processes in the SPND cause the mass sensitivity to be much lower for Co-based SPNDs than for Rh-based
SPNDs. Over time the transmutation product 60 Co builds up, gradually producing a radioactive product
that may require special handling when the SPND is removed from the reactor core. Also, 60 Co is a beta
particle emitter with T1/2 = 5.27 years. The result is an increasing background signal with neutron fluence.
Some modern systems have compensating electronics for this gradual increase in background current while
shielded emitter designs have been proposed to limit the number of 60 Co beta particles emerging from the
emitter [Goldstein and Todt 1979].
Platinum has also been investigated as an emitter material [Shields 1973; Lynch et al. 1977], although the
name SPND is misapplied because it is not strictly a neutron detector.27 However, for completeness the use
of Pt as an emitter is discussed here. Instead of neutron activation, Pt emitters rely directly upon gamma-ray
interactions. Further, it is actually desirable that it is insensitive to neutrons because the measurement relies
on gamma-ray interactions. Platinum is a candidate because of it high atomic number (78), relatively low
average neutron absorption cross section (∼ 10 b), and high density (21.45 g cm−3 ). Gamma rays interact
in the emitter by either photoelectric or Compton events, which eject energetic electrons from the emitter.
As with the Co-SPND, gamma rays also interact in the insulator and the collector, giving rise to opposing

27 Shields named them “self-powered flux detectors”.


Sec. 17.10. Time-of-Flight Methods 887

current to the emitter current. Also as with the Co-SPND, the measured current is the net response from
the summed emitter and collector currents. A Pt-SPND has a prompt response to power step changes in a
reactor and reportedly a higher sensitivity than Co [Goldstein and Todt 1979]. However, it is assumed with
Pt-SPNDs that the gamma-ray flux scales proportionally with the neutron flux, which may not be exact,
especially at the reactor core boundaries.
There are additional drawbacks to using Pt as an emitter material; mainly, it does in fact respond to both
gamma-rays and neutron interactions [Lynch et al. 1977]. Neutron capture by 195 Pt, with a thermal-neutron
capture cross section of σγ = 29b, produces prompt high-energy gamma-rays of 5.9 MeV and 6.1 MeV
[Tuli 1997]. The thermal neutron capture cross section for 196 Pt is relatively small at σγ = 0.4b; however,
the resonance integral capture cross section is σI,γ = 5 b, producing predominantly 333 keV and 356-keV
gamma rays [Lone et al. 1981]. Finally, neutron capture by 198 Pt, with σγ = 3.7b and σI,γ = 56b, produces
a undesirable beta particle emission response (T1/2 = 30.8 min). Lynch et al. [1977] report that as much as
55% of the total signal can result from neutron interactions for some emitter geometries, but also provide a
method to discern between neutron and gamma-ray induced signals.

17.10 Time-of-Flight Methods


Another method used to measure the energy of a neutron involves the use of timing circuitry (covered in
Chapter 22) with which the speed of a neutron is recorded. Suppose that a finite package of neutrons is
released from a source, where the starting time gate is linked in coincidence with a neutron detector some
distance from the source. Then the detector can be connected to record pulse height events as a function
of arrival time. Usually this time spectrum is recorded with a multichannel analyzer where the channels are
increments in time. For low energy neutrons, relativistic effects are negligible. The arrival time is a direct
measure of the speed, or energy, 
d mn
t= =d , (17.116)
v 2E
where t is the time duration between pulse initiation and detection, v is the neutron velocity, d is the distance
between the neutron source and detector, mn is the neutron mass, and E is the neutron energy. Given any
velocity v or energy E, it becomes clear from Eq. (17.116) that the time spread increases with distance d.
To produce a simulated pulse from a neutron source, a device named a chopper is generally used.28 The
first such devices consisted of a large spinning disk with open spaces for neutrons to pass through, while
the remaining portions of the disk were composed of a neutron absorber [Amaldi et al. 1935, Frisch and
Sorenson 1935, Dunning et al. 1935b, Fink 1936]. The device described by Frisch and Sorenson [1935] was
a 50-cm diameter wooden wheel that was 2 cm thick, and relied on neutron collisions with protons in the
wood to attenuate slow neutrons. The upgraded design by Dunning et al. [1935b] used an aluminum wheel
with portions blocked by Cd. In the Dunning et al. [1935b] design, and also the Fink [1936] design, a second
stationary Cd collimator, adjacent to the neutron detector, was used downstream from the rotating disk to
accept only those neutrons that emerged from chopper opening.
An improved design, shown in Fig. 17.45 and conceived by Fermi et al. [1947], has a series of parallel slots
arranged in a rotating cylinder (or drum). These collimator slots need not be voids, but are usually thin
plates of Al clamped between layers of Cd. Notably, the Cd works well for low-energy neutrons with energies
below approximately 0.5 eV, but because neutron absorption reduces tremendously above 0.5 eV, it is less
effective for higher energies of neutrons. The chopper is rotated at high speeds, where the slots align with
the source every half-rotation of the chopper. When the slots are aligned with the neutron stream, a burst
of neutrons from the source passes through the chopper and heads towards the detector. The start time is

28 These devices were originally named velocity selectors, but by the mid-1950s the name chopper had been largely adopted.
888 Slow Neutron Detectors Chapt. 17

measured by producing a gate signal when the chopper is aligned with the detector, often performed with a
magnetic or optical actuator. If it is assumed that the uncertainty in d is relatively small, the uncertainty
in the energy calculation can be approximated with Eq. (17.116)
 2 1/2 
dE 2 Δt 8 Δt 3/2
ΔE = (Δt) = 2E = E , (17.117)
dt t m d

where Δt is the uncertainty in the flight time.


As shown in Section 17.7.5, the interaction rate in 1
in Cd 1
16 in Al
a 1/v absorbing detector is independent of neutron en- 32
o n
ergy for slow neutrons with energies in the 1/v region. ro
ta
t i

Hence, the number of counts recorded as a function of


time yields a measure of the energy distribution of slow
neutrons emerging from the chopper. To reduce neu-
incident 5
tron scattering effects, a beam collimator that is either neutrons 1 16 in

evacuated or backfilled with 4 He or oxygen should be


positioned between the chopper and the detector (see
Fig. 17.46).29
Seidl et al. [1954] describe a fast neutron chopper 1 Al
in steel
32
with eight pairs of collimated channels on a relatively 2 in
0.004 in - 0.008 in Cd

large wheel (30-inch diameter). The device was de-


signed for neutron energies ranging between 10 eV up Figure 17.45. Cross section view of the chopper design
to 10 keV, where the stopping material is phenolic lam- from Fermi et al. [1947].
inate. The chopper was designed to operate at about 12000 rpm with a temporal emission distribution that
appears approximately as an isosceles triangle with FWHM of 0.7 μs. The distance between the chopper
and a bank of 10 BF3 detectors was 20 meters, between which was a large plastic helium-filled “balloon”.

moderator
collimator collimator

chopper beam stop

reactor He-filled tube

shield detector
d

Figure 17.46. One method to arrange a TOF neutron


energy measurement from a nuclear reactor.

29 One of the earliest applications of neutron beam choppers was to measure the neutron lifetime. An alternative method is to
place neutrons in a cryogenic bottle, whose walls are perfect neutron reflectors, and measure how many remain after a period
of time. At first both methods gave slightly different results, a difference in the mean lifetime of 9-s that persists to this day
and is well outside experimental errors. One explanation could be a neutron decay mode that does not produce a proton, in
which case the beam method would overestimate the neutron lifetime.
Problems 889

PROBLEMS
1. For an infinite homogeneous medium with weak sources and absorption, the flux of thermal neutrons
in thermal equilibrium with the thermal motion of the ambient atoms is given by the Maxwellian
distribution 
2πn 2
φM (E) = 3/2
Ee−E/kT .
(πkT ) mn
Here n is the total neutron density, k is Boltzmann’s constant, T is the neutron temperature (K), and mn
is the neutron mass. Show (a) the most probable energy (the energy at which φM (E) has a maximum
is ET ≡ kT ) and (b) the average energy is 2ET = 2kT .

2. Other forms of the Maxwellian distribution include


(a) neutron number density energy distribution
2πn √ −E/(kT )
nM (E) = Ee
(πkT )3/2

(b) neutron flux velocity distribution

mn 3/2 2
φM (v) = 4πn v 3 e−mn v /(2kT )
2πkT
(c) neutron number density velocity distribution

mn 3/2 2
nM (v) = 4πn v 2 e−mn v /(2kT )
2πkT
Sketch these three distributions and that of Problem 1. Find the average and most probable speed or
energy for each.

3. Determine the thermal-neutron absorption length for a 3 He gas-filled detector pressurized to 4 atm.
If the detector has a diameter of 1 inch (2.54 cm), what is the maximum attenuation for a beam of
neutrons intersecting perpendicular the tube cross section?

4. You have a 10 BF3 detector built from a 25-mm diameter (I.D.) Al tube, backfilled with 0.2 atm of 10 BF3
and 2 atm of Ar gas. If a 0.5 cm diameter thermal-neutron (2200 m s−1 ) beam intersects the detector
mid-section, what is the expected intrinsic thermal-neutron detection efficiency?

5. Given a thermal-neutron beam (0.025 eV) intersecting a 10-mm-thick sample of CLYC:Ce, determine
the intrinsic thermal-neutron detection efficiency of the CLYC:Ce sample. If the natural Li is replaced
with 96% enriched 6 Li, what is the new thermal-neutron detection efficiency?

6. A monoenergetic beam of neutrons is normally incident on a thin sheet of material. Confining your
attenuation to a single atom in the material, how long must you wait, on the average, before a neutron
interacts with the atom? The beam intensity is 1010 neutrons cm−2 s−1 and the total microscopic cross
section for the atoms is 10 barns.

7. Determine the intrinsic (2200 m s−1 ) thermal-neutron detection efficiency for a neutron beam normally
incident on the front surface of a Si diode coated with 1.5 microns of 96% enriched 10 B. In the coating,
the range of the 4 He ion is 2.3 microns and that for the Li ion is 0.8 microns. Assume absorption in the
contact layer is negligible.
890 Slow Neutron Detectors Chapt. 17

8. Sketch the expected pulse height spectrum from a thermal-neutron beam intersecting the midpoint of
a P-10 gas-filled detector with inner walls coated with (first) 1 micron 90% enriched 10 B over which a
10-micron layer of 95% enriched 6 LiF layer has been applied.

9. Explain the possibilities and limitations of operating 3 He and 10 BF3 detectors as ion chambers, Geiger-
Müller counters, or proportional counters. What practical consideration dictates using the latter (pro-
portional) operation?

10. The sensitivity or efficiency of a BF3 tube or a boron lined tube decreases with use because of the
burnup of the 10 B. If such a tube is exposed to a constant thermal flux φ, show that the tube sensitivity
decreases in time as exp[−σa φt], where σa is the absorption cross section for 10 B.

11. A young engineer decided that it was time for change with present day neutron detectors and designed
a 10 BF3 proportional tube with 6 LiF-coated walls. Sketch the expected pulse height spectrum if the
LiF is very thin. Sketch the expected pulse height spectrum if the LiF is as thick as the maximum
range of the highest energy reaction product from the 6 Li(n,t)4 He reaction. Discuss advantages and
disadvantages of the design.

12. Why can’t the counting efficiency of a boron-lined proportional counter be increased indefinitely by
simply increasing the coating thickness?

13. The government of the rogue nation Haides seeks to develop an atomic bomb. But enriching its abundant
natural uranium reserves to extract 235 U is beyond the technical and financial abilities of the nation.
However, Haides’ chief nuclear scientist, Prof. Lou Cipher, thinks there is another way to acquire suffi-
cient 235 U. Because fission chambers contain 93% enriched U, they could provide an easy, commercially
available, alternative to obtaining the needed 235 U. One such chamber with an active cylindrical region
of length 35 cm and diameter of 18 cm has a 93% enriched UO2 coating of thickness 0.015 μm. Prof.
Cipher has learned from his spies that a reflected sphere of 15 kg of 93% enriched 235 U is needed for a
nuclear weapon. How many fission chambers must Haides acquire?

14. In what situations is a 3 He tube preferred over a BF3 tube for counting thermal neutrons?

15. What is the expected activity of an 1 cm2 Au foil 500 microns thick irradiated in a thermal neutron
beam of 106 cm−2 s−1 for 30 minutes?

16. Although the gold foil activation technique is designed for thermal neutron measurements in which the
neutrons have a Maxwellian energy distribution, it can also be used in other situations involving slow
neutrons. For example, a neutron diffractometer is sometimes used to extract neutrons of (almost) a
single energy from the neutrons with thermal Maxwellian distribution leaving a beam port of a nuclear
reactor. This monodirectional monoenergetic beam can then be used to calibrate a slow neutron detector
as described in Sec. 17.6.5. Modify the analysis of Sec. 17.7 to obtain an expression for the activation
of a gold foil in such a beam to determine the intensity (flux) of the monoenergetic beam.

17. Show that Eq. (4.146) for a relativistic heavy charged particle reduces to Eq. (17.28) for a non-relativistic
heavy ion.

18. Derive Eq. (17.112).

19. Consider an SPND with 103 Rh as the emitter with an atom density of No . Let the subscripts “1” and
“2” refer to 104m Rh and 104 Rh, respectively. The atom density, decay constant, and activation cross
References 891

section are denoted by Ni (t), λi , and σi , respectively, i = 1, 2. A new SPND is inserted into a reactor
operated at a constant flux of φo . Show that the buildup to equilibrium of the two daughters is given
by
No σ1 φo
N1 (t) = (1 − e−λ1 t ),
λ1
and
No φo (σ1 + σ2 )
N2 (t) = − [1 − e−λ1 t ].
λ2

20. Consider the 103 Rh SPND of the previous problem. Show that the transients from equilibrium as φo → 0
at t = 0 are given by
No φo σ1 −λ1
N1 (t) = e ,
λ1
and " #
σ1 + σ2 −λ2 σ1 : −λ1 t ;
N2 (t) = No φo e + e − e−λ2 t
λ2 λ2 − λ1

21. Given a Rh SPND operating continuously in a BWR for 6 months at a thermal-neutron flux of 1014
cm−2 s−1 , what is the expected percent decrease in observed current?

22. A beam chopper is used to select neutrons with speeds of 300 m/s. After traveling down a 30-m beam
line, 3.40% fewer neutrons reached the detector than left the chopper. Estimate the mean lifetime of
neutrons.

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Instrum. Meth., A460, 1–14, (2001). Nucl. Instrum. Meth., A336, 226–231, (1993).

VAN EIJK, C.W.E., A. BESSIÉRE, AND P. DORENBOS, “Inorganic WILPERT, T., “Boron Trifluoride Detectors,” Neutron News, 23,
Thermal Neutron Scintillators,” Nucl. Instrum. Meth., A529, 14–19, (2012).
260–267, (2004). WU, J-W, A. WELTZ, M. KOIRALA, J.J-Q. LU, R. DAHAL, Y.
DANON, AND I.B. BHAT, “Boron-10 Nanoparticles Filled Silicon
VAN EIJK, C.W.E., J.T.M. DE HAAS, P. DORENBOS, K.W.
Trenches for Thermal Neutron Detection Application,” Appl.
KRAM̈ER, AND H.U. GÜDEL, “Development of Elpasolite and
Phys. Lett., 110, paper 192105, 5 pages, (2017).
Monoclinic Thermal Neutron Scintillators,” Conf. Rec. Nucl.
Sci. Symp., paper N12-3, pp. 239–243, Puerto Rico, Oct. 23–29, YAMAGUCHI, S., “Edge Effect of Thin Lithium-Glass Scintilla-
(2005). tors,” Nucl. Instrum. Meth., A274, 573–578, (1989).
Chapter 18

Fast Neutron Detectors


These results, and others I have obtained in the course of the work, are very difficult to explain
on the assumption that the radiation from beryllium is a quantum radiation, if energy and
momentum are to be conserved in the collisions. The difficulties disappear, however, if it
be assumed that the radiation consists of particles of mass 1 and charge 0, or neutrons.
Sir James Chadwick

18.1 Detection Mechanisms


Because interaction cross sections for neutrons in the epithermal to fast region are generally relatively
small (except in narrowly defined resonance regions) compared to thermal-neutron cross sections, detectors
designed for fast neutrons must rely on alternative approaches to those traditionally used for thermal-neutron
detectors that rely on a select few isotopes with large reaction cross sections. An additional difficulty is
encountered in the detector design if the goal is to distinguish between thermal and fast neutrons.
Fast neutron detection can be divided into three basic methods. First, fast neutrons can be detected
by moderating them into the thermal or epithermal energy region for which a traditional thermal-neutron
detector can be used as the sensor. Second, fast neutrons, upon scattering, can introduce recoil atoms into a
detecting medium, which is either attached to the detector or is part of the detector material. Third, a fast
neutron may undergo in the detector material a nuclear reaction that can, by some means, be distinguished
from those produced by thermal neutrons.

18.1.1 Neutron Moderation and Scattering


A common method of detecting fast neutrons is through neutron moderation. This technique places low
atomic number materials close to a traditional thermal-neutron detector. Neutrons scatter in the moderator
material and lose energy with each scatter, until, ultimately, they lose enough energy such that absorption
in the thermal-neutron detector becomes likely.
The kinematics of inelastic neutron scattering are discussed in Sec. 4.3.4. In this chapter only elastic
scattering (Q = Δ = 0 and γ = 1/A) is considered and the results of Chapter 4 are considerably simplified. In
particular, the interrelationships among the cosine of the scattering angles are repeated here for convenience.1
From Eq. (4.47)
1 + Aωc
ωs = √ , −1 ≤ ωc ≤ 1. (18.1)
1 + 2Aωc + A2
From Eq. (4.48)

ωc = −(1 − ωs2 )/A + ωs 1 − (1 − ωs2 )/A2 , −1 ≤ ωs ≤ 1. (18.2)

1 Herethe subscript c and s refer to the center-of-mass and laboratory systems, respectively. The scattering angle is θi and its
cosine is ωi = cos θi , i = c, s.

897
898 Fast Neutron Detectors Chap. 18

For the special case of A = 1 in which ωs ≥ 0 this result reduces to ωc = −1 + 2ωs2 , which implies θc = 2θs .
The cosine of the angle of the recoil nucleus for elastic scattering is given by Eq. (4.55) as

1 − ωc
ωr = = sin(θc /2), 0 ≤ ωr ≤ 1, (18.3)
2
and, from Eq. (4.54), the recoil energy of the nucleus is

T 2A 4A
= (1 − ωc ) = ω2. (18.4)
E (1 + A)2 (1 + A)2 r

This result indicates that the maximum energy transfer occurs when the laboratory scattering angle of the
recoil nucleus θr is 0, or when θs = θc = π.
For a given incident neutron energy E, any one of ωs , ωc , ωr , E  , or T is independent, i.e., specification
of one determines values of the other parameters. Because scattering is azimuthally symmetric about the
direction of the incident neutron in polycrystalline materials, the singly differential scattering cross sections
in terms of the different scattering parameters are related by

dσs (E, ωc ) dσs (E, ωs ) dσs (E, E  )  dσs (E, T )


2πdωc = 2πdωs = 
dE = − dT. (18.5)
dΩc dΩs dE dT

Notice the minus sign in the last term, an indication that as T decreases, ωc , ωs , and E  all increase.

Example 18.1: Determine the maximum fractional energy transfer for neutron scattering off H and 4 He.

Solution:
From Eq. (18.4) for hydrogen, in which A = Z = 1,

T 4A cos2 θr 4(1) cos2 (0)


= = = 1.
E (1 + A)2 (1 + (1))2

This result shows that the total energy E of the neutron can be transferred to the proton in a single collision,
provided θs = π. For elastic scattering from 4 He,

T 4A cos2 θr 4(4) cos2 (0)


= = = 0.64,
E (1 + A)2 (1 + (4))2

which indicates that a maximum of 64% of the neutron energy can be transferred to a 4 He nucleus in a
single scatter.

18.1.2 Multiscattered Neutrons Table 18.1. Elastic slowing down param-


eters. Data are from [Lamarsh 1966].
Although a single scatter with hydrogen can transfer a fast neu-
tron to the thermal region, generally several scatters are required. Nucleus Mass No. ξ
1H 1 1.000
On average, the number n of scatters required to degrade a neu-
H2 O 0.920
tron with initial energy Eo to a lower energy E is [Lamarsh 2H (or D) 2 0.725
1966] D2 O 0.509
1 Eo Be 9 0.209
n = ln , (18.6) C 12 0.158
ξ E
O 16 0.120
Sec. 18.2. Detectors Based on Moderation 899

where ξ is2  
(A − 1)2 A+1
ξ =1− ln . (18.7)
2A A−1
For example, using the data of Table 18.1, to thermalize a neutron from 2 MeV to 1 eV requires 14.51, 15.77,
28.5, and 91.83 scatters in H, H2 O, D2 O, and C, respectively.

18.1.3 Absorption
Epithermal and fast neutrons can also be absorbed in materials, although the probability of this is usually
lower than that observed for slow neutrons in most materials. However, fast neutrons must pass through the
absorption resonance energies of materials as they slow down. The rate at which these slowing neutrons are
absorbed is defined by the resonance integral which, for a 1/E slowing down spectrum is defined as
 Emax
dE
I= σa (E) . (18.8)
ECC E

where Emax is the maximum neutron energy or energy at which absorption resonances can be resolved. Thus
the fast neutron absorption rate in a foil, for example, is given by Eq. (17.82).
There are several select isotopes that absorb neutrons only at energies above a specific threshold energy.
Discussion of these threshold reactions is deferred to later in this chapter where foil activation methods are
discussed.

18.2 Detectors Based on Moderation


A simple method used to detect fast neutrons is to provide a means to moderate the neutrons and slow
them to thermal energies so that a traditional thermal-neutron detector can be used, such as a 3 He gas-filled
detector. The methods may include simply detecting the presence of neutron or may include complicated
unfolding algorithms used to determine the neutron energy spectrum. Some of these moderation detection
methods are described in the following sections.

18.2.1 Bonner Spheres


A small thermal-neutron detector is placed in the center of a sphere of high density polyethylene (HDPE).
Fast neutrons entering the HDPE sphere lose energy through scattering and, thus, increase the probability of
interacting in the thermal-neutron detector. Usually the thermal-neutron detector is a 6 LiI:Eu scintillator,
although 10 BF3 and 3 He gas-filled detectors have been used [Rotondi and Geiger 1968; Goldhagen 2011], as
well as activation foils [Thomas et al. 2002a].
The spheres can be obtained commercially in a set of different diameters, often referred to as a Bonner
sphere set, named after one of the pioneering authors of the method [Bramblett et al. 1960; Bonner 1961].
A set of commercial Bonner spheres usually has between 6 to 10 different sizes so that several different
measurements of the neutron field can be made including one with the bare detector. The main components
to a Bonner sphere detector are shown in Fig. 18.1, along with a depiction of a few fast neutron trajectories.
Also shown in Fig. 18.1 is a photograph of a commercial Bonner sphere set.
For a small sphere, there is little moderation and it is unlikely that a high energy neutron loses enough
energy to be efficiently detected by the neutron detector should it enter that sphere. As the size of the

2A neutron of energy E has a lethargy u(E) ≡ ln(Emax /E) where Emax is the maximum energy of a neutron in a system. As
E decreases, u increases, i.e., the neutron moves more lethargically, and hence the name lethargy. Here ξ is the average gain
in lethargy per scatter averaged over all scattering angles.
900 Fast Neutron Detectors Chap. 18

Figure 18.1. (left) Depiction of the main Bonner sphere components. Also shown
are several possible neutron trajectories along which some neutrons scatter out of
the Bonner sphere, some neutrons are absorbed by the Bonner sphere, and some
neutrons are detected by the 6 LiF:Eu scintillator. (right) The Ludlum model 42-5
is a commercial Bonner sphere set and rack with 6 different Bonner sphere sizes.
Courtesy of Ludlum Measurements.

sphere is increased, the moderation becomes more pronounced for fast neutrons, but overly so for low energy
neutrons. Hence, epithermal neutrons may lose too much energy before reaching the detector and be absorbed
in the moderator. As the size of the sphere increases further, moderated neutrons with sufficient range to
reach the detector may miss it entirely and either be absorbed in the moderator or even escape from the
Bonner sphere. Overall, the detector response is a complex function of how the neutrons enter a sphere, the
detector absorbing medium (such as 6 Li or 10 B), the detector absorber mass thickness, the Bonner sphere
size, and the distance in air (or other medium) between the neutron source and the detector. Thomas and
Alevra [2002b] discuss many of these points in a review on the operation of Bonner spheres for neutron
spectroscopy [see also the results of Burgett et al. 2009].
Slow neutrons interact readily with the thermal-neutron detector and, therefore, need no moderation.
For each sphere under test, neutrons interacting in the spheres undergo scattering reactions that lead to
some moderation. Thermal neutrons may be completely absorbed in even the smallest moderator sphere,
usually 2 inches (5 cm) in diameter, and thus go undetected. However, slow neutrons in the low eV range
have a relatively high probability of being detected because this sphere is optimized for 1 eV neutrons as
can be seen from Fig. 18.2. The next size up is optimized for a slightly higher neutron energy, and so on
for the remaining spheres. Most sets have a 12-inch (30.5 cm) diameter sphere as the largest size, although
some sets have spheres as large as 18 inches (45.7 cm).
The response function for the ith sphere, Ri (E), such as those shown in Fig. 18.2, gives the average
number of counts per incident neutron of energy E. The response function depends on the size and type
of thermal-neutron detector at the center of each sphere and how the sphere is illuminated by neutrons.
For example, a 1-in diameter incident neutron beam has a different response function than that for broad
beam illumination. In such cases the response functions depend on what portion of a sphere is illuminated
Sec. 18.2. Detectors Based on Moderation 901

Figure 18.2. Calculated response functions for different sized Bonner spheres
over a thermal-neutron detector (6 LiI scintillator). Data extracted from Jacobs
and van den Bosch [1980].

and the intersecting location on the sphere (centered, off-centered, etc.). Likewise, response functions for a
point neutron source near the sphere differs from that for the source placed far from the sphere. Most often
reported response functions are for spheres uniformly illuminated by a plane parallel beam of monoenergetic
neutrons. In this case Ri (E) gives the average count rate per unit intensity of the beam, i.e., counts per
neutron cm−2 .
For a particular neutron energy, the probability that the detector records a count can be determined with
Monte Carlo techniques [Braga and Dias 2002; Bedogni et al. 2007]. The response functions calculated by
Monte Carlo simulations have associated statistical errors and are also obtained for only discrete incident
neutron energies. These results are then subjected to some smoothing procedure to make each Ri (E) a
smooth continuous function of E.
The neutron field incident on a Bonner sphere is characterized by its energy-dependent intensity or flux
φ(E) (cm−2 MeV−1 s−1 ), which here is assumed to be monodirectional and constant in time over a sphere.
The detector response function Ri (E) is the count rate obtained with the ith sphere per unit incident beam
intensity of energy E. Hence the count rate observed the ith of N spheres is given by the Fredholm equation

 Emax
ci = Ri (E)φ(E) dE, i = 1, . . . , N, (18.9)
Emin

where Emax and Emin are the maximum and minimum neutron energies in the neutron spectrum. Given the
N measured ci and the response functions Ri (E), the unfolding problem is to solve these equations for the
neutron energy spectrum φ(E).
Neutron spectra are usually plotted versus the logarithm of energy. Thus to accurately fit the data, the
unfolding problem is better handled in terms of the logarithm of energy. Equivalently, the neutron lethargy
902 Fast Neutron Detectors Chap. 18

u can be used. The lethargy is defined as


 
Emax
u ≡ ln , (18.10)
E
whose derivative with respect to energy is simply
du 1
=− . (18.11)
dE E
The maximum lethargy umax corresponds to the minimum energy, and Eq. (18.9) can be written as
 umax
ci = du R(u) φ(u), i = 1, . . . , N, (18.12)
0
where R(u) = R(E(u)) and φ(u) = E(u)φ(E(u)).
Typically, the Bonner sphere response functions are determined by using Monte Carlo methods, which
with cubic spline or some other method for smoothing result in a set of curves such as those shown in
Fig. 18.2. These response function calculations can be verified by using known fast neutron sources (see
Tables 5.6 and 5.7 for examples of neutron sources). The next step in unfolding an unknown spectrum is
to convert the Fredholm equations, Eq. (18.9) or Eq. (18.12), into linear algebraic equations by using some
numerical quadrature method. The simplest such discretization is to assume φ(E) is constant over each
energy interval formed by a contiguous grid of energies (or lethargies) Ej and Ej+1 , j = 1, . . . , M . Thus,
Eq. (18.9) or Eq. (18.12) are transformed to

M
ci = Ri,j φj , i = 1, . . . , N. (18.13)
j=1

where M is the total number of assigned flux groups. In matrix form these equations can be written
compactly as
c = R•φ (18.14)
where c and φ has elements ci and φj and the response matrix R has elements Rij .
Many unfolding methods and algorithms have been developed since the introduction of the Bonner
sphere method by Bramblett et al. in 1960. Some of these unfolding techniques take various types of neutron
source spectra into consideration, and can identify the most probable source [Matzke 2002; Goldhagen 2011].
However, the method is time consuming and relatively cumbersome because between 6 or more measurements,
depending on the set, must be made with long enough measurement times to ensure reasonable counting
statistics. Further, during the measurement process, the user assumes that the neutron flux environment
is unchanging. Finally, although the result is a neutron spectrum, it is usually of relatively low resolution.
Hence, Monte Carlo codes and archived data are often used as a comparison to the measured results to
determine the most probable neutron source (or spectrum) [Thomas and Alevra 2002b].
If the number of Bonner spheres N is greater than or equal to the number of energy groups M , then
Eqs. (18.9) can be solved outright. The resolution of the solution increases with the number of Bonner
spheres (and energy groups). However, if the number of energy groups exceeds the number of Bonner sphere
measurements, then one must deal with an underdetermined set of equations, which, generally, have an
infinity of solutions, most of which are physically unrealistic such as negative or complex fluences. Two basic
approaches for solving Eqs. (18.13) have evolved over time [Ryan 1998]. The oldest is one based on some
iteration scheme wherein some initial spectrum guess is modified to give better agreement with Eqs. (18.9).
The second and more recent approach is to add constraints (such as positivity) to the possible solutions and
obtain as many equations as there are unknowns so as to regularize the unfolding problem. The bases of
both of these approaches are outlined below.
Sec. 18.2. Detectors Based on Moderation 903

The Iterative Method of Doroshenko


An iterative algorithm developed by Doroshenko et al. [1977] is used in many commercial unfolding codes
for the Bonner sphere system and is the basis of comparison for the Backus-Gilbert method in this study.
The Doroshenko method utilizes a simple recursion relationship to infer the approximate solution from
the measured data. The algorithm requires an initial guess of the neutron spectrum Φ0 , which produces
estimated count data given by c0i = ri •φ0 , where ri is ith row vector of R for moderator i. Successive
estimates of the flux φk+1 are found by iterating the relation
N =N 
 ri  ri
φ k+1
=φ k
, k = 0, . . . , kmax , (18.15)
ck
i=1 i
c
i=1 i

where kmax is the maximum number of iterations and cki = ri •φk . Essentially, this method attempts to bring
the estimated count data cki into agreement with the measured count data ci by adjusting the estimated
neutron spectrum φk .
A measure of error  in the iteration is the root mean squared difference between the estimated and
measured count rates
1  (cki − ci )
N 2
2
 = . (18.16)
N i=1 ci
Although this outcome does not actually reflect the error between the true and measured solutions,  does
reflect the convergence rate of the method. In most problems  decreases rapidly and approaches a fixed
value, making  a poor cutoff criterion for iteration. Therefore, it is more useful to observe the change, for
the k-th iteration, δk = k − k−1 , which approaches a uniform value more slowly than .
Provided that the response functions ri and the estimate φ0 are both positive, positivity of solutions is
guaranteed by Eq. (18.15). Good numerical stability is demonstrated for solutions that are similar to the
initial estimate. Most importantly, the method gives places more importance on regions where Ri is large, or
where each detector combination is the most sensitive. Unfortunately, the method is limited in its ability to
handle unknown neutron spectra, where no estimate of φ0 is possible. Because φ0 is modified by Eq. (18.15)
so as to agree with the measured count rates, it has a strong influence on the final solution φkmax . Secondly,
the cutoff criterion kmax is an arbitrary parameter that also depends on φ0 . For small values of kmax the
estimated solution closely resembles φ0 . For large values, numerical instabilities yield non-realistic results.
The Regularization Method
The neutron spectrum φ(u) can be recovered by minimization principles, using numerical methods as outlined
in Press et al. [1992]. To utilize a priori information in calculating a solution, one might choose two positive
functionals A[φ] > 0 and B[φ] > 0, such that φ can be determined by minimization of A[φ] or B[φ]. A can
be chosen to estimate the accuracy of the solution, and B to estimate some fixed solution property, such as
smoothness.
One obvious functional to minimize that quantifies how good a possible solution φ  is the χ2 statistic
⎡ ⎤2
N 
M
χ2 = ⎣ci − j ⎦ ,
Rij φ (18.17)
i=1 j=1

where the variances are neglected in this brief discussion. In many regularization schemes A is taken as χ2 .
For the Bonner sphere problem (and many other inverse problems) M N (more unknowns than equations)
there are an infinity of solutions some of which make χ2 very small, if not zero. However, such solutions
 To
almost always oscillate widely and otherwise are physically unrealistic (negative or complex values of φ).
904 Fast Neutron Detectors Chap. 18

obtain realistic solutions, some additional information or constraints on φ (contained in the functional B)
are specified.
Thus, the goal is to minimize A[φ] subject to the constraint that B[φ] = b. The method of Lagrange
multipliers allows this type of minimization problem to be solved by introducing a multiplier μ. The Lagrange
functional to be minimized is given by

L = A[φ] + μ1 (B[φ] − b), (18.18)

The minimum of Eq. (18.18) is found by setting its first derivative with respect to φ equal to zero,

∂ ∂
{A[φ] + μ1 (B[φ] − b)} = (A[φ] + μ1 B[φ]) = 0. (18.19)
∂φ ∂φ

Alternately, B[φ] can be minimized subject to the constraint that A[φ] = a using Lagrange multiplier μ2 .

∂ ∂
{B[φ] + μ2 (A[φ] − a)} = (B[φ] + μ2 A[φ]) = 0. (18.20)
∂φ ∂φ
In either case, the inverse problem is changed to

minimize A + μB. (18.21)

As μ = μ1 = 1/μ2 varies between 0 and ∞, the solution φ(μ) varies along a trade-off curve between
minimizing A (small μ) and minimizing B (large μ). Thus any solution along this trade-off curve can be
interpreted as (1) minimizing A subject to constraint B = b, (2) minimizing B subject to constraint A = a,
or (3) minimizing the sum A + μB.
A benefit of this minimization scheme is that a unique solution φ can be obtained even where A[φ] is
degenerate. The general theory and several methods for regularizing underdetermined problems are given
by Press et al. [1992]. Application of this method to unfolding Bonner sphere data is given by Ryan [1998]
who used the Backus-Gilbert approach in which A and B are chosen so as to maximize the stability of the
 Reginatto et al. [2002] used the maximum entropy method in which B is taken as the negative
solution φ.
of the entropy, or negentropy, and the inverse problem becomes


M
 +μ
minimize χ2 (φ) φj ln(φj ). (18.22)
j=1

18.2.2 REM Counters


The REM counter is a special Bonner sphere that is 10 inches (25.4 cm) in diameter, and is a common
device used to measure neutron dose equivalent H. The detector used with many commercial units is a
3
He detector embedded in the ball, the entire detector/sphere combination attached to a handheld survey
unit. The reason for the chosen 10-inch diameter is that the detector response is close to that for an average
human dose equivalent [Hankins 1962; Bramblett et al. 1960].
Hankins [1962, 1965] compares the calculated response of a 10-inch Bonner sphere with a central 6 LiF:Eu
detector with the inverse radiation protection guide (RPG) response.3 This comparison is shown in Fig. 18.3.

3 Thisquantity is more frequently called the fluence-to-dose conversion factor or dose response function. It is the dose rate per
unit neutron flux in units of dose per neutron.
Sec. 18.2. Detectors Based on Moderation 905



!#$
 


*+


&''&(#)

!"#$%

,-&'


           

   

Figure 18.3. Calculated responses from a 10-inch Bonner sphere rem counter compared to (the
then) recommended inverse RPG curve. Data are from Hankins [1965]. Also shown are results
from the International Commission on Radiological Protection (ICRP) and the National Bureau
of Standards (NBS) which is now the National Institute of Standards and Technology (NIST).

At energies below 200 keV, the instrument overestimates the neutron dose by as much as a factor of 5 for
some energies. At energies above 7 MeV, the instrument severely underestimates the neutron dose. For
these reasons, Hankins [1965] recommends that neutron dosimetry with the basic 10-inch Bonner sphere be
restricted to the 200 keV to 7 MeV range. However, modifications to the rem counter design permits the use
of smaller diameter spheres, usually ranging between 7 inches and 9 inches, to obtain results that adequately
match the inverse RPG curve for energies between thermal and 7 MeV.
A cylindrical neutron dosimeter instrument based on the same concept as the Bonner sphere was in-
troduced by Andersson and Braun [1964]. The detector is designed with 10 BF3 gas-filled detector with a
diameter of about 30 mm and an active length of 60 mm placed inside cylinders of polyethylene. There
is an inner annulus of polyethylene with a 0.63 inch (16 mm) wall thickness encapsulated by a perforated
5-mm-thick blanket of boron-loaded polyethylene. Surrounding the entire configuration is another annu-
lus of polyethylene with a 2.56 inch (65 mm) wall thickness and length of 9.6 inches (244 mm). Lastly, a
43-mm-thick plug of polyethylene is placed inside the outer annulus in front of the 10 BF3 detector. The
detector design has several basic features in common with the first long counter designs (discussed in the
next section).
Although the response to neutrons above 7 MeV is similar to that determined by Hankins [1965] for
the 10-inch Bonner sphere, the energy region below 200 keV gives a better fit to the RPG curve. However,
this response improvement comes at the expense of a heavier instrument, reportedly 8.5 kg. These types
of detectors are commercially available, which still use the basic cylindrical design and gas-filled neutron
detector.4 In some cases, the 10 BF3 detector has been replaced with a 3 He detector. Modern designs have

4 The Canberra SNOOPY and the Thermo-Fisher Wendi-2 (see Fig. 18.4) are based on the Andersson-Braun design.
906 Fast Neutron Detectors Chap. 18

Figure 18.4. The Thermo Fisher model FHT Figure 18.5. The Ludlum model 12-
762 Wendi-2 Wide-Energy neutron detector is 4 is a commercial 9-inch spherical rem
a commercial unit based on the Andersson- counter based on the Leake design. Repro-
Braun design. Reproduced with permission from duced with permission from Ludlum Mea-
Thermo Fisher Scientific. surements, Inc.

replaced the boron loaded polyethylene with a boron doped synthetic rubber layer. The introduction of heavy
elements sheets into the Andersson-Braun design have extended the useful energy range of the instrument.
Mares et al. [2002] report a variation that includes a lead layer encapsulating a perforated boron doped
rubber layer, both surrounding the polyethylene encapsulated 10 BF3 detector, a change that extends the
neutron detection range beyond 1 GeV. This increase in response is due to (n,xn) fast reactions in the lead.
Leake [1966] modified the Andersson-Braun design to improve the detector response with respect to the
RPG curve while reducing the weight of the instrument. The first such modification was styled much like
the Hankins [1962] device, but included concentric spheres around the 10 BF3 detector. A smaller Cd-covered
polyethylene sphere encapsulated the detector, while a larger 8.2 inch diameter polyethylene concentric ball
surrounded the device. The Cd covered ball suppressed the over-response of neutrons in the low energy
region (below 0.5 eV) while reducing the overall weight by eliminating boron-loaded polyethylene sections.
Overall, the device response is similar to the inverse RPG curve and weighs only 5 kg.
Another improvement reported by Leake [1968] was to replace the 10 BF3 detector with a spherical 3 He
detector. The change reduced background gamma-ray counts while improving the efficiency, and the entire
device weighed approximately 6.6 kg. This Leake detector, as it became known, was for many years a
standard commercially available instrument.5 Because of changes made by the International Commission on
Radiological Protection (ICRP) in their fluence-to-dose conversion factors, minor alterations in the Leake
design have been implemented over the years [Leake 1999; 2004] to remain in compliance. These commercial
units are usually designed to follow the inverse RPG curve from thermal neutron energies up to 7 MeV. They
also detect neutrons up to 10 MeV, although the results are not dose equivalent. Additional modifications
have been explored to increase the detection range of neutron energies. For instance, Hsu et al. [1994] report
the responses of a lead shell surrounding the detector, within various polyethylene ball sizes, yielding up to

5 For instance, Ludlum Measurements, Inc., produces a wide variety of Leake-style handheld units (see Fig. 18.5).
Sec. 18.2. Detectors Based on Moderation 907

a 5 times increase in sensitivity to 800 MeV neutrons. The use of Cu, Pb, and W to extend the neutron
energy range was also explored by Burgett et al. [2009].

18.2.3 Long Counter


Early measurements of the number of neutrons emitted from fast sources were performed by Amaldi and
Fermi [1936] and Amaldi et al. [1937] by immersing a neutron source in a water bath and measuring the
thermal-neutron signal at various locations in the bath. The technique was later adopted by O’Neal [1946]
to measure the neutron energy spectra of different photo-neutron sources. The radiation detector used in
the former (Amaldi et al. 1937) case was an ion chamber, while activation foils were used in the latter
(O’Neal) case. Although the methods proved useful, the inconvenience of the water bath and the time
consuming approaches led Hanson and McKibben [1947] to seek a practical and portable solution, called the
long counter.
The first long counter was based on the concept introduced by Amaldi and Fermi [1946], but replaced the
water bath with paraffin and the detector with a 10 BF3 gas-filled proportional counter. The original device
had a 1-inch diameter 10 BF3 detector, with a sensitive length of 8 inches, centrally inserted into a 12-inch
long cylinder of paraffin. Slow neutrons could enter the detector front (one end of the 10 BF3 tube) or the
adjacent paraffin. The escape probability for slow neutrons from the paraffin is high near the front of the
device but decreases for higher energy neutrons that penetrate further into the paraffin cylinder. Overall, the
probability of a neutron being moderated and absorbed somewhere along the length of the 10 BF3 detector
is nearly independent of the neutron energy so a flat energy response is achieved. Through experimentation,
it was determined that an 8-inch-diameter paraffin cylinder produced the most uniform counting response
from a wide spectrum of neutron energies.
The design was modified to exclude neutrons scattered in air surrounding the device by including a shield
surrounding the inner portion. The shield consisted of a B2 O3 blanket and another thick encapsulating
blanket of paraffin, as shown in Fig. 18.6. Holes were drilled into the inner paraffin cylinder to assist with
the detection of the lower energy fast and epithermal neutrons. Further, the 10 BF3 detector active length
was 10.5 inches. The basic design of the shielded long counter, as developed by Hanson and McKibben
[1947], is still used today, although there have been modifications and improvements over the years [Allen
1960; De Pangher and Nichols 1966; East and Walton 1969].
McTaggart’s device [see Allen 1960] implemented a few design modifications to optimize the long counter
response. The holes were drilled deeper to a length of 6 inches. McTaggart’s experiments demonstrated that
the flatness of the long counter response would deteriorate if the detector was pushed from its flush position
further into the paraffin moderator (see Fig. 18.7). Hence, the 10 BF3 detector was inserted such that the
front end was flush with the paraffin moderator. Also, a 1.5-inch-long boron sleeve was placed over the
10
BF3 detector with the front edge 3 inches from the paraffin front face. Finally, the inner moderator length
was extended to 14 inches, while the outer moderator length was extended to 20 inches. These changes
produced a flat response within 5% for neutrons with energies of 25 keV to 5 MeV. The optimized shielded
long counter of McTaggart has become known as the standard long counter.
Other changes, such as those described by De Pangher and Nichols [1966] rendered additional improve-
ments. A reported problem with the standard long counter was the response reproducibility between different
counters [Tagziria and Thomas 2000]. De Pangher and Nichols [1966] sought to remedy this problem with
many changes to the standard long counter design aimed at regularizing the components. The paraffin was
replaced with high density polyethylene (HDPE), the B2 O3 glass thermal neutron shield was replaced with
boron-loaded polyethylene, and the outermost housing was fabricated from aluminum. The 1-inch diameter
holes were replaced with an annular trench and thicker Cd shields were positioned on both ends of the de-
vice. According to Marshall [1970], the De Pangher design, also called the precision long counter, rendered
reproducible results superior to the standard long counter. Harvey et al. [1976] report that the precision
908 Fast Neutron Detectors Chap. 18

casing of 0.05” sheet iron

paraffin paraffin
B2O3

paraffin paraffin
Al sleeve
1” diameter holes

1.675” 3.5” 8” 9” ~15”


Cd cap
BF3 detector ceresin
(wax)

3” 7” 3.5” 2.5”

16.5”

Figure 18.6. The original shielded long counter design as described by Hanson and McKibben [1947]. Depicted are
(left) a cross section and (right) front view.


 !"
$!"


 !"

%
&' !())
 !


#!"


   
   

Figure 18.7. The response of McTaggart’s long counter as a function of the axial
location of the 10 BF3 detector end (as x) from the paraffin face. Also shown is a
comparison between the optimized McTaggart detector (x = 0 inch) and the original
Hanson-McKibben detector. Data are combined from Allen [1960].

long counter response was relatively independent of neutron energy. Various researchers have calibrated both
the standard long counter and the precision long counter [Slaughter and Rueppel 1977; Hunt and Mercer
1978; Tagziria and Thomas 2000], and found that both long counter designs perform well for neutrons with
energies up to about 10 MeV.
Another design called the modified long counter and reported by East and Walton [1969] replaced the
10
BF3 detector with five 3 He gas-filled proportional counters in an attempt to increase the overall neutron
detection efficiency. This detector has the usual cylindrical shape, but has incorporated many changes to
Sec. 18.2. Detectors Based on Moderation 909

the moderator. The inner moderator is HDPE with a diameter of 9 inches, while the outer moderator is
boron-loaded paraffin. Instead of 8 holes drilled into the inner moderator, there are 12 holes, each 1-inch
in diameter and 3.5 inches deep in the HDPE. Although the hole pattern is symmetric, they are no longer
on a single radial axis, but rather staggered around a radius of approximately 3.5 inches. Another torus
of HDPE, approximately 0.75 inch thick, covers most of the hole openings on the device. The resulting
device did show improved detection efficiency with a near constant value of 11.5 ± 0.5% for neutron energies
between 25 keV and 4 MeV. However, because the Q value of the 3 He(n,p)3 H is much lower than the Q
value of the 10 B(n,α)7 Li reaction, the authors report that background gamma-ray interference is worse than
with a standard long counter, and recommend the standard long counter for neutron measurements in a high
gamma-ray field.

18.2.4 Directional Neutron Spectrometer


First introduced by Oakes et al. [2010], and Cooper et al. [2011; 2012], the directional neutron spectrom-
eter is a relatively new device that uses the fundamental concept of the Bonner sphere. However, instead
of having to change several spheres, one for each measurement, the unit has numerous slices of moder-
ators arranged as a cylinder. Between each moderator slice is an array of compact thermal-neutron de-
tectors, usually of the MSND variety (see Sec. 17.5). A single spectral measurement is performed with
all detectors in place, and does not require the removal or replacement of moderators [Oakes et al. 2013].
The output data is processed and template- display Al housing
matched to the most probable neutron source
from a library containing hundreds of environ- detector power supply
front electronics board
ment conditions and neutron source spectra.
A depiction of the first prototype detector ar-
rangement is shown in Fig. 18.8. possible
neutron
The initial sectioned neutron spectrometers trajectories
had up to 20 HDPE layers with a fourplex ar-
ray of dual-stacked MSNDs between each layer,
and a bare MSND array at the front of the stack HDPE Cd sheet MSND
array
[Cooper et al. 2011]. In later experimental ver-
sions, the small fourplex array was increased to Figure 18.8. The basic arrangement of a sectioned neutron spec-
as many as 108 detectors per layer with 30 mod- trometer from Cooper et al. [2011, 2012].
erator layers to give a total of 3240 detector channels [Hoshor et al. 2015]. With a mass of nearly 50 pounds
(22.7 kg), this large device pushed the limits of portability. Commercial models are considerably lower in
weight and have approximately 16 MSNDs per layer. The total number of detectors varies with the number
of moderator slices, usually between 7 to 12 slices per unit. The response of an eight-layer device to an AmBe
and 252 Cf source is shown in Fig. 18.9. Commercial handheld devices range in weight from approximately
8 pounds (3.62 kg) to 20 pounds (9.1 kg). The detector can rapidly identify the neutron spectrum from
numerous fast neutron sources under a variety of environmental circumstances [Hoshor et al. 2015; 2017].
This neutron spectrometer also doubles as an imaging device, capable of locating the general direction(s)
of the fast neutron source(s). Although the direction finding algorithm can be complicated, it fundamentally
operates by tallying counts from the MSNDs in the total array and identifying an imaginary vector drawn
from the lowest average count rate per device to the highest average count rate per device. The vector is
used to point towards the most probable source location and is usually accurate to within a few degrees.
910 Fast Neutron Detectors Chap. 18

Figure 18.9. Calculated relative response functions for an eight-layer sectioned neutron
spectrometer. Also shown for comparison are energy spectra from 252 Cf and AmBe
neutron sources. Data from Hoshor et al. [2015].

18.2.5 Other Moderated Detectors


There are other types of detectors that take advantage of the moderation detection method. In fact, prac-
tically any thermal-neutron detector can be inserted into a moderator material, usually HDPE, to improve
overall sensitivity to fast neutrons. The gas-based neutron detectors described in Chapter 17 are commonly
inserted into HDPE blocks to improve fast neutron responses. Along with the gas-filled devices already
described in this chapter, other examples include moderated 3 He detectors reported by Kamboj et al. [1978],
and moderated 10 BF3 detectors reported by Barrett et al. [1969] and Sekharan et al. [1976]. The system
reported by Kamboj et al. [1978] has several 3 He detectors in a layered block of polyethylene with the goal of
producing another neutron source calibration device similar to the long counter. They report a linear neutron
energy response between 2.1 and 4.5 MeV. The system described by Barret et al. [1969] has numerous BF3
detectors embedded in a large single block of paraffin all positioned radially about a neutron source. The
method is based on the analysis by Thies [1963] and provides a relatively flat response for neutron energies
ranging from 30 keV to 5 MeV. A similar 4π system reported by Sekharan et al. [1976] was designed to
measure the cross sections for various neutron producing reactions. The performance of moderated 6 Li-foil
detectors were described by Nelson et al. [2014; 2015]. High densities of MSNDs have been inserted into
moderators with reportedly similar performance as high-pressure 3 He gas-filled detectors [Ochs et al. 2017].

18.3 Detectors Based on Recoil Scattering


Detectors based on recoil scattering rely on the recoil atoms transferring energy to a detection device. For
gas detectors, the recoil ion generates electron-ion pairs that can be measured as the output. Scintillators
generally rely either on scattered recoil ions that are a part of the scintillator to fluoresce the scintillator,
such as an organic scintillator, or rely on recoil products entering and fluorescing an adjacent scintillator,
Sec. 18.3. Detectors Based on Recoil Scattering 911

Figure 18.10. Elastic scattering cross sections for many materials used for
recoil detectors. Data are from [ENDFPLOT 2017].

such as a ZnS:Eu scintillator. Semiconductors can also be used, whose constituent elements in the material
recoil and produce electron-hole pairs. From Eq. (18.4), it becomes clear that more energy is transferred
per scatter from low A recoil materials than from high A materials. Consequently, most detectors based on
recoil ion scatter are manufactured from the lighter elements. The neutron elastic scattering cross sections
for several isotopes used for recoil detectors are shown in Fig. 18.10.

Differential Scattering Cross Sections


The differential scattering cross section quantifies how likely a neutron is to scatter into some new direction
from its initial direction. With this information the energy and angular distribution of a recoil nucleus can
be determined. This topic is explored in this section.
Of course all scattering cross section measurements are performed in the laboratory coordinate system
but, primarily for historical reasons, scattering information was often converted to the center of mass system,
fitted to a sum of Legendre polynomials, and the resulting expansion coefficients were then archived in the
early cross section libraries. To use such data, the results, upon extraction, had to be reconverted to the
laboratory system. This cumbersome approach was used because generally much less scattering data needed
to be saved. For low energy neutron scattering in which a compound nucleus is formed, which is at rest in
the center of mass system, the subsequent neutron decay occurs isotropically because information about the
incident neutron direction is “forgotten” during the relatively long lifetime of the compound nucleus. Thus,
the differential scattering cross section would appear almost constant in the center of mass system and only
one Legendre coefficient had to be saved.
Today, computer memory and data storage is much less expensive and data from scattering in the
laboratory system can readily be archived. The many cross section libraries available from nuclear institutions
around the world, now generally have a mixture of scattering data in the two coordinate systems and one
must be careful in the use of retrieved scattering data as to which coordinate system was used for the data.
912 Fast Neutron Detectors Chap. 18

The conversion of the differential scattering cross section from the laboratory system into the center of
mass system is found from Eq. (18.5) as
dσs (E, ωc ) dσc (E, ωs ) dωs
= , (18.23)
dΩc dΩs dωc
where ωs = cos(θs ) and ωc = cos(θc ). Differentiation of Eq. (18.1) with respect to ωc and substitution of the
result into Eq. (18.23) gives
dσc (E, ωc ) dσs (E, ωs ) A2 [A + cos(θc )]
= . (18.24)
dΩc dΩs [1 + 2A cos(θc ) + A2 ]3/2
Energy Distribution of the Recoil Nucleus
The probability that a neutron of initial energy E transfers energy into dT about T to the scattering nucleus
is
1 dσs (E, T )
P (E, T ) dT = dT, (18.25)
σs (E) dT
which, from Eq. (18.5), can be written as
 
1 dσs (E, ωc ) 2πdωc
P (E, T ) dT = − dT. (18.26)
σs (E) dΩc dT
Differentiation of Eq. (18.4) with respect to ωc gives
dωc (1 + A)2 2
=− =− , (18.27)
dT 2AE (1 − α)E
where α = (A − 1)2 /(A + 1)2 . Substitution of this result into Eq. (18.26) gives the energy distribution of
the recoil nucleus
1 dσs (E, ωc ) 4π
P (E, T ) = , 0 ≤ T ≤ (1 − α)E. (18.28)
σs (E) dΩc (1 − α)E
Thus the ideal pulse height spectrum from a single scatter is proportional to the differential scattering cross
section in the center of mass coordinate system.

Example 18.2: In some cases scattering in the center of mass system is isotropic, i.e., dσs (E, ωc (E, T ))/dΩc
is simply σs (E)/(4π). For this case, derive an expression for dσs (E, T )/dT .

Solution:
From Eq. (18.2) one finds
dωc −2
=
dT (1 − α)E
so that, from Eq. (18.5),
dσs (E, T ) dσs (E, ωc ) 4π
=− ,
dT dΩc (1 − α)E
which upon substitution of dσs (E, ωc (E, T ))/dΩc  σs (E)/(4π), gives the desired result
dσs (E, T ) σs (E)
 .
dT (1 − α)E
Sec. 18.3. Detectors Based on Recoil Scattering 913

18.3.1 Gas Detectors Based on Recoil Scattering


The most popular backfill gases are low mass gases, usually 1 H, 3 He, 4 He, and CH4 . The reaction cross
sections for these gases are shown in Fig. 18.11. Except for 3 He detectors, detectors filled with these gases
all respond in similar manners. All gas-based
recoil detectors function with a gas com- 10 4
posed, at least in part, of a low Z material.
The usual candidates include pure hydrogen,
10 3
CH4 , and helium, although other hydroge- 3 3
He(n,p) H

Cross Section (barns)


nous gases can work. Energetic neutrons
scatter from the detector gas and transfer 10 2
some kinetic energy to the recoiling atom, 1 1
H(n,n) H
as described by Eq. (18.4).6 Typically these
10 1
detectors are designed as a type of propor- 3 3
He(n,n) He
tional counter, although gridded ion cham-
bers can also work. Gas recoil detectors can 10 0
4
He(n,n) He
4

in principle detect relatively low energy scat-


ters, yet the practical lower energy threshold
is near 20 keV [Ferguson 1960]. The detector 10 -1
10 -8 10 -7 10 -6 10 -5 10 -4 10 -3 10 -2 10 -1 10 0 10 1
cavity should be of adequate dimensions be- Neutron Energy (MeV)
yond the expected range of the recoiling ions
in order to reduce wall effect distortions in Figure 18.11. Neutron reaction cross sections for 1 H, 3 He, and 4 He.
the pulse height spectrum. The ion ranges Data are from [ENDF VIII 2018].
can be reduced by increasing the gas pressure; however, as reported in Chapter 10, increasing the gas pres-
sure reduced the charge carrier velocity and can reduce the response proportionality. At operating pressures
up to 20 atm, these detectors can respond to neutron energies up to 20 MeV.
The possibility of carbon scattering is high in a CH4 chamber, and the differential scatter cross section
for carbon is not at all uniform. Also, the maximum energy transfer for carbon is only 28%, significantly less
than proton recoil contributions. Further, the pulse height spectrum of the recoil energy becomes even more
complicated when the proton recoil wall effect is included. Detectors based on the use of 4 He are a commercial
alternative. These detectors do not have the complications of multiple nuclides, but the differential scattering
cross section is not isotropic. Hence, the pulse height spectrum is not a simple step function, although the
endpoint energies for monoenergetic neutrons should be near 64% of the initial neutron energy (see Example
18.1).
Typical commercial units are pressurized between 0.526 atm (400 torr) up to 10 atm (7600 torr). Advan-
tages of the high pressure tubes include increased detection efficiency and extended energy range. However,
the operating voltage must also be increased, usually to several thousand volts. Further, the gamma-ray
background is higher for the pressured recoil detectors. Detectors with lower pressures respond faster to
neutrons, require much lower operating voltages (often less than 1000 volts), and suffer less background con-
tamination. However, the recoil particle ranges are longer such that the recoil range increases approximately
inversely proportional to the gas pressure. Because of the importance of hydrogen as a moderator and a
source of recoil ions, these detectors are considered first.

6 The recoil atom may be an ion having lost one or more shake-off electrons. As the speed of the recoil atom increases above
the speed of K-shell electrons, it becomes increasingly likely the recoil atom has shed one or more electrons.
914 Fast Neutron Detectors Chap. 18

Proton Recoil Detectors with Hydrogen


Neutron scattering from hydrogen is nearly isotropic in the center-of-mass coordinate system. Hence, the
differential scattering cross section dσsH (E, ωc )/dΩc for hydrogen can be well approximately as σsH (E)/(4π)
for neutron energies well beyond 20 MeV. From Eq. (18.28) with α = 0 for H, the ideal recoil energy
distribution P (E, T ) is a constant or step function ranging from T = 0 to T = E, the incident neutron
energy.
n
To preserve energy information, these detectors are
n 1 generally fashioned as cylindrical proportional counters.
3
p
The interaction efficiency for a given neutron energy can
p be estimated by a simple exponential approximation,

p
p (E) = 1 − exp[−NH σsH (E)], (18.29)
p
2 where NH is the atomic density of hydrogen in the detec-
n
tor, σsH is the elastic scatter cross section of hydrogen,
Figure 18.12. Three possible ways in which neutrons can and w is the detector effective width. Three possible
interact in a 1 H2 gas detector. neutron trajectories are depicted in Fig. 18.12. For tra-
jectory 1, multiple scatters cause the neutron to pass nearly all of its energy to hydrogen in the detector. For
trajectory 2, the neutron escapes the detector after leaving partial energy behind. Finally, in trajectory 3,
the neutron imparts all of its energy to a proton in a single scatter. Because the range of energetic protons
in hydrogen gas is relatively long, the recoil protons often strike the wall or enter the dead regions of the
counter (see end effect in Sec. 17.3.1) so as to produce a type of wall effect. These effects distort the pulse
height spectrum from the expected step function. Although hydrogen seems to be an obvious choice for a
recoil detector gas, it is usually not used in spectroscopic applications because of the wall-effect distortions.
Several types of gas-filled recoil detectors use high purity hydrogen gas, which would be an obvious choice
considering the previously reviewed kinematics for scattering from 1 H. Shown in Fig. 18.13 are the differential
elastic scattering cross sections in the laboratory system for different incident neutron energies on 1 H. The
results of combining the differential scattering cross section for hydrogen in Fig. 18.13 at a few select energies
with the conversion of Eq. (18.24) are shown in Fig. 18.14. Note that when A = 1 that Eq. (18.2) reduces
simply to θc = 2θs . It is seen that the differential elastic scattering cross section for hydrogen is remarkably
constant (isotropic) at all scatter angles in the center of mass system, i.e., dσs (Ec , ωc )/dΩc = σs (E)/4π.
With A equal 1 and isotropic center-of-mass scattering, Eq. (18.28) reduces to P (E, T ) = 1/E, 0 ≤ T ≤
E so the expected pulse height spectrum from hydrogen scattering is simply a rectangular step function
terminating at T = E, the energy of the incident neutron. There are a few notable points when dealing with
1
H as the scattering medium. First, the neutron scatter angle in the laboratory system is restricted between
angles π/2 ≤ θs ≤ 0, i.e., there is no neutron backscatter. Second, the neutron can transfer its entire energy
to the recoil proton. Third, the probability of scattering through any angle between π ≤ θc ≤ 0 in the
center-of-mass system is practically constant.
Although it would seem that 1 H is the ideal gas for a recoil spectrometer, there are some problems
with the use of 1 H as the recoil gas. The range of the recoil proton can be significant in hydrogen gas,
approximately 163 ± 2.13 mm for a 2 MeV proton in 2 atm of 1 H2 gas. Even if the detector is oriented
longitudinally to the fast neutron source, there is still a significant probability that the recoil proton collides
with the chamber wall before expending all of its energy, thus producing a wall effect (see Section 17.3.1).
The wall effect can be reduced by increasing the gas pressure, but this remedy comes at the expense of longer
response time and increased gamma-ray background. Recall from Chapter 10 that gamma-rays primarily
interact in the detector shell and not directly in the gas. Hence, the energy deposited by photoelectrons or
Compton electrons entering the gas increases approximately linearly with gas pressure. Consequently, the
LLD must be increased as the pressure is increased and, hence, reduces the epithermal neutron response
Sec. 18.3. Detectors Based on Recoil Scattering 915

Figure 18.13. The laboratory system 1 H differential scattering cross sections in barns
per steradian (dσ/dΩ) for several incident neutron energies. Data are from [ENDF VIII
2018].

Figure 18.14. The center-of-mass system 1 H differential scattering cross sections con-
verted from data of Fig. 18.13 with Eq. (18.24). That the resulting plots are lines parallel
to the abscissa is confirmation that scattering is isotropic in the center-of-mass system.
916 Fast Neutron Detectors Chap. 18

of the detector. Further, the total interaction cross section is relatively constant over a large energy range
from 0.1 eV up to approximately 10 keV (see Fig. 18.10). Beyond 10 keV, the elastic scattering cross section
decreases, dropping from 18 barns at 20 keV eventually to 0.48 barn at 20 MeV. To counter this reduction
in the microscopic cross section at fast neutron energies, the pressure in the detector container may be
increased; however, the interaction efficiency for gamma-rays increases as well. Many of these effects are
discussed in detail in the literature [Snidow and Warren 1967; Gold and Bennett 1968; Benjamin et al. 1968;
Weise et al. 1991].

Proton Recoil Detectors with Non-Hydrogen Gases


There are other gases of interest for proton recoil detectors, mainly CH4 and 4 He. Note that 3 He gas can
also be used, but because it also has a considerable neutron absorption reaction cross section, is covered in
a latter section. To overcome the range problem, in part, methane can be used instead of pure hydrogen
[Fink et al. 1980], or at least a partial pressure of methane can be added to the detector chamber [Bennett
1962]. Consequently, the recoil proton range is reduced and allows the detector to respond to higher energy
neutrons. For instance, the range of a 2-MeV recoil proton in 2 atm of methane is 39.7 ± .6 mm, less
than a quarter of that in 2 atm of 1 H2 . Benjamin et al. [1968] describe a spherical proportional counter
backfilled with P-10 gas that has reduced wall and end effects. However, neutron scattering from carbon,
which transfers at most only 28% of its energy per scatter, distorts the pulse height spectrum [Bennett
1962]. Although the carbon may leave some residual energy in the gas that appears in the low energy region
of the spectrum, it is the energy reduction of the scattered neutron that distorts the high energy cutoff.
The scattered neutron may subsequently interact with a hydrogen atom, and, because of its reduced energy,
produces recoil protons also of reduced energy, thereby shifting the spectrum to lower energies.
The use of 4 He as a proportional gas in neutron spectrometers was suggested many decades ago, perhaps
initially by Baldinger et al. [1938]. The use of 4 He gas is attractive because the range of an energetic 4 He
ion is significantly lower to that of a proton of equal energy. The effect is enhanced because a 4 He recoil
ion can carry at most only 64% of the initial fast neutron energy, and the proportional gas (4 He) has a
higher stopping power than H2 gas. From Eq. (18.4), the maximum scatter energy of a 4 He recoil ion from
a 2 MeV neutron is found to be 1.28 MeV, and the range of this recoil ion in 2 atm of He is 17.5 ± 0.37
mm, over 9 times less than in 2 atm of 1 H2 gas. Further, the total microscopic elastic scatter cross section
for 4 He surpasses that of 1 H at approximately 800 keV. Hence, the interaction efficiency is higher in a 4 He
proportional counter than in a 1 H2 counter with an equal atomic density. For neutron energies up to 15
MeV, it is necessary to increase the stopping power of recoil protons by adding another noble gas. Because
Xe and Kr are more susceptible to gas impurities, and there is a natural radioactive isotope 85 Kr that can
add to the background, a common choice is to use a large percentage of Ar. Birch [1988] reports on a 40%
Ar/60% 4 He mixture for the measurement of 15 MeV neutrons.
Unlike 1 H, the differential cross section for 4 He is not uniform at all center-of-mass scattering angles.7
Consequently, the pulse height spectrum becomes somewhat complicated. The lab system and center-of-
mass system differential cross sections for 4 He are shown in Figs. 18.15 and 18.16, respectively. The results
of using the data of Fig. 18.16 combined with Eqs. (18.4) and (18.28) are shown in Figs. 18.17 and 18.18,
which show the idealized features expected from 4 He proportional gas detector. The pulse height spectral
distortions imposed by variations in charge carrier collections times, wall effect, and detector dimensions
have been modeled by various research groups [for example Atwater 1972; McDaniel and Hungerford 1979;
Weyrauch et al. 1998]. Atwater [1972] provides a model that includes the wall effect, gas pressure, and
Gaussian smearing to produce a more realistic recoil spectrum for a 4 He detector and is shown in Figs. 18.19
and 18.20. The similarity of the results of Figs. 18.17 and 18.18 to those of Figs. 18.19 and 18.20 are apparent.

7 In fact, 1 H is the only nuclide that possesses this property in the MeV energy range.
Sec. 18.3. Detectors Based on Recoil Scattering 917

Figure 18.15. The laboratory system 4 He differential scattering cross sections in barns
per steradian (dσ/dΩ) for several energies. Data are from [ENDF VIII 2018].

Figure 18.16. The center-of-mass system 4 He differential scattering cross sections in


barns per steradian (dσ/dΩ) for several energies. The graphs were generated from the
data of Fig. 18.15 and Eq. (18.24).
918 Fast Neutron Detectors Chap. 18

Figure 18.17. The ideal pulse height distribution for Figure 18.18. The ideal pulse height distribution for
recoil ions scattered from fast neutrons. The ordinate recoil ions scattered from fast neutrons. The ordinate
is P (E, T ) and is plotted as a function of the 4 He recoil is P (E, T ) and is plotted as a function of the 4 He recoil
energy. Curves are labeled with initial neutron energy. energy. Curves are labeled with initial neutron energy.

Figure 18.19. Calculated differential pulse height Figure 18.20. Calculated differential pulse height
spectrum in 8 atm 4 He from monoenergetic neutrons. spectrum in 8 atm 4 He from monoenergetic neutrons.
Data from Atwater [1972]. Data from Atwater [1972].

Birch [1988] reports that the proton background from (n,p) reactions in the steel wall of the chamber
become considerable for neutron energies above 10 MeV. To mitigate this problem a 0.5-mm-thick lead
liner is inserted into the gas-chamber. Weyrauch et al. [1998] further develop a model for commercial 4 He
proportional counters and give a variety of comparisons of theoretical to measured results. It is interesting to
note that, although 4 He gas-filled recoil detectors work adequately as neutron spectrometers, the problems
with charge collection are greatly mitigated if the device is instead used as a gas scintillation detector [Jebali
et al. 2015].

18.3.2 Unfolding the Recoil Energy Spectrum


If a fast neutron detector is to be used for neutron spectroscopy to determine the energy dependent flux
φ(E) of the neutrons incident on the device, the signals recorded by the instrument must be processed to
obtain an estimate of φ(E). None of the fast neutron detectors described in this chapter directly give φ(E)
and some unfolding of the measured data must be made to obtain the energy information. Briefly mentioned
Sec. 18.3. Detectors Based on Recoil Scattering 919

here is how unfolding a measured recoil energy spectrum can be approached. The measured recoil energy T
is related to the incident neutron flux φ(E) by a Fredholm integral equation
 Emax
T = R(T, E)φ(E) dE, 0 ≤ T ≤ Tmax , (18.30)
0

where Emax is the maximum neutron energy, Tmax = (1 − α)Emax is the maximum recoil energy, and R(T, E)
is the spectrometer response function which gives the probability of observing a recoil energy T per unit
intensity of an incident monoenergetic (E) neutron beam. The response function, as a first approximation,
is given by Eq. (18.28). But an accurate determination of R(T, E) requires Monte Carlo simulations to
account for multiple scatters, wall and end effects, statistical fluctuations, non-linearities in the scintillators,
and non-ideal behavior of the electronics.
To obtain φ(E) from Eq. (18.30), the integral equation (like that for a Bonner sphere) is first converted
to a set of linear algebraic equations. This conversion can be performed by several methods. The simplest
method is to form a contiguous energy grid E1 = 0, E2 , . . . Ei , Ei+1 , . . . , EI+1 = Emax with Δi ≡ Ei+1 − Ei .
Similarly, the recoil energy range (0, Tmax ) is split into J contiguous energy intervals Δj . Typically, the Δj
are equi-width and are the interval widths of the MCA channels used to record the recoil energies.
Equation (18.30) can be written as
I 
 Ei+1
T = R(E, T )φ(E) dE. (18.31)
i=1 Ei

Integration over the jth recoil energy interval gives


 Tj+1 I 
 Ei+1  Tj+1
T dT ≡ Tj = dE dT R(E, T )φ(E) j = 1, . . . , J , (18.32)
Tj i=1 Ei Tj

where Tj is the measured count rate in channel j of the MCA spectrum of the recoil energy spectrum. If the
flux φ(E)  φi is constant in each neutron energy interval Δi , then Eq. (18.32) becomes


I
Tj = Rji φi , j = 1, . . . , J , (18.33)
i=1

where the elements of the response matrix are


 Ei+1  Tj+1
Rji = dE dT R(E, T ). (18.34)
Ei Tj

Hence, J linear algebraic equations for the I unknowns of the φi are obtained. If the recoil atoms and
incident neutrons use the same energy grid, then I = J and the solution to Eq. (18.34) can be obtained by
standard means. Birch [1988] describes two unfolding methods to determine the incident neutron spectrum
from the 4 He recoil spectrum, namely matrix inversion and iterative unfolding. He reports better resolution
for the iterative unfolding method, especially after differentiating the pulse height spectrum and the response
functions.

18.3.3 Scintillators Used in Recoil Neutron Scattering


The basic physics regarding scintillation detectors are described in Chapters 12 and 13 and are not repeated
here, except perhaps for some clarification. Both inorganic and organic scintillators are used for fast neutron
920 Fast Neutron Detectors Chap. 18

detectors. The inorganic scintillators can be used as adjacent devices to a recoil medium, such as a hydroge-
nous material, and which fluoresces from the interactions of recoil ions. Organic scintillators are usually
deployed as a combined recoil-fluorescence detector, in which proton (or carbon) recoils from fast neutrons
in the organic compound subsequently fluoresce the scintillator. Already discussed in Chapter 13, organic
compounds suffer non-linear light yield as the differential energy deposition increases. A few of the detectors
and configurations that primarily use recoil reactions as the detection mechanism are briefly described in
the following sections.
Response of Organic Scintillators
Organic scintillators, discussed in Section 13.3, are compositions of hydrogen, carbon, and some with other
elements such as nitrogen. Proton recoil scattering is nearly isotropic in the center-of-mass system, and the
resulting pulse height spectrum for monoenergetic incident neutrons resembles closely a simple step function
that extends from zero energy up to the incident neutron energy E. Further, from Eq. (18.4), a fast neutron
may impart all of its energy to a proton recoil in a single scatter, but at most only 28% of its energy to a
carbon atom with a single scatter. Consequently, the response function from an organic scintillator deviates
from the ideal step function. In fact, there are multiple factors that transform the observed pulse height
spectrum, including the characteristic non-linear response of organic scintillators, statistical fluctuations,
multiple scattering, edge effects, and directional asymmetry [Swartz and Owen 1960].
The Ideal Case There are numerous organic scintillators that contain only hydrogen and carbon atoms,
such as the crystalline organics anthracene and stilbene, numerous plastics, and many liquids. Notably, many
popular organic fluors contain nitrogen. However, for simplicity, the discussion is limited here to organic
scintillators that contain only H and C.
With the definition used by Swartz and Owen [1960], efficiency is the ratio of the number of recoil protons
to incident neutrons. The molecular density Nhc of the organic scintillator is
ρNa
Nhc = , (18.35)
A
where ρ is the mass density, and Na and A have the usual designations of Avogadro’s number and the
substance’s molecular weight. The atomic densities of hydrogen and carbon can be expressed, respectively,
as
ρNa ρNa
NH = fH Nhc = mH 2 and NH = fC Nhc = 12mC 2 , (18.36)
A A
where fH and fC are, respectively, the mass fractions of hydrogen and carbon per molecule. Here mH and
mC are, respectively, the masses of hydrogen and carbon per molecule, which, to a good approximation, are
the number of hydrogen and carbon atoms per molecule. Multiplication by the microscopic scattering cross
section gives the macroscopic scattering cross sections,

ΣH = σH NH and ΣC = σC NC . (18.37)

The expected efficiency for proton recoil interactions involving a single scatter is,

N1 (E0 , ) ΣH
1h = = [1 − exp [−(ΣH + ΣC ) ]] , (18.38)
N0 (ΣH + ΣC )

where N1 (E0 , ) is the number of recoil protons produced by a single scatter of a neutron with initial energy
E0 in a scintillator of length and N0 is the fluence of neutrons impinging on the scintillator. Equation (18.38)
indicates that, provided that the crystal is of adequate length, a sufficiently high efficiency can be expected.
In practice, large volumes of organic detector are impractical, mainly because the absorption efficiencies
Sec. 18.3. Detectors Based on Recoil Scattering 921

of gamma rays and charged particles also increase and ultimately interfere with the recoil signal. The
use of various discrimination methods can reduce background interference. These methods include pulse
height analysis, pulse shape analysis, coincidence (or anticoincidence) counting, capture gating with loaded
scintillators, and the selection of clever scintillator physical dimensions to reduce energy deposition from
energetic electrons. The ideal pulse height spectrum can be defined by a step function,
$
N1 (E0 , )/E0 Tp ≤ E0
N (Tp ) = . (18.39)
0 Tp > E0

Unlike gas detectors which measure the energy distribution of the recoil atoms directly, scintillators
produce a light yield distribution from the energy deposited by the recoil atoms. It is much more difficult to
extract the energy distribution of the incident neutrons from the pulse height spectrum of the light output
than from the pulse height distribution of the energy from recoil atoms as produced by a gas detector.
Further, there are various distortion effects that alter the ideal differential pulse height spectrum of light.
Some of these effects include non-proportional light yield, statistical fluctuations, carbon scattering, multiple
proton scatters, recoil protons escaping the detector, and in some cases direction asymmetry in light yield.
The combined effects cause the distortion from the ideal case Fig. 18.21(a) to that shown in Fig. 18.21(f).
A brief discussion of these effects follows.
Scintillator Non-linearity The non-linearity of the light output L of an organic scintillator is given by
Eq. (13.36), which with slight changes in notation, can be written as8

dL  dT /dx
A
= , (18.40)
dx 1 + kB dT /dx

 is the quenching parameter,


where k is the probability that an exciton is lost to a non-radiative transition, k B

A is a proportionality constant, and L is the luminous output.
The variable P (same energy units as L) for pulse height is introduced as P = L/A,  such that Eq. (18.40)
becomes
dP 1
= . (18.41)
dT 
1 + k B dT /dx
 is known, then numerical integration of Eq. (18.41) yields values of P . In the ideal case, k B
If k B  is zero and
P = T ; hence P would also be a rectangular step function for proton recoils. Also, for energetic electrons,
dT /dx is small and P = T once again. However, for recoil protons, scintillation quenching can have a
significant impact on the luminescent yield and the quenching parameter cannot be ignored. The number of
recoil protons with energy between Tp and Tp + dTp is defined as N (Tp )dTp , where Tp is the initial energy
of the recoil proton. The pulse height spectrum of the light output is written as N (P )dP so that

dTp
N (P ) = N (Tp ) . (18.42)
dP
Typically a solution to Eq. (18.42) is obtained through numerical methods and unfolding algorithms
[Slaughter and Strout 1982]. However, in some cases, empirical formulas fit to measured data can simplify
the evaluation of Eq. (18.42). For instance, the light yield L or P can be modeled as a power function of the

8 Herethe empirical constants are denoted by A  and B to avoid confusion with the symbols without the accent. Also the
charged particle energy is denoted by T instead of E to avoid confusion with the neutron energy.
922 Fast Neutron Detectors Chap. 18

effect of
non-proportional
ideal step light yield ideal step
function function

Counts per Channel


Counts per Channel

(a) (b)
Channel Number (Energy) E0 Channel Number (Energy) E0
effect of multiple
effect of proton scattering
ideal step ideal step
carbon scattering
function function
Counts per Channel

Counts per Channel


0.72 E0

effect of
statistical
fluctuations

(c) (d)
Channel Number (Energy) E0 Channel Number (Energy) E0

edge effect combined effects ideal step


ideal step
distortion function
function
Counts per Channel
Counts per Channel

(e) (f)
Channel Number (Energy) E0 Channel Number (Energy) E0

Figure 18.21. Representative pulse-height distortions from neutron scattering in an


organic scintillator. (a) The ideal case with no distortions; (b) non-linear light yield; (c)
statistical fluctuations; (d) carbon scattering and multiple proton scattering; (e) edge
effects; and (f) the resulting spectrum from the combined effects.

recoil energy, usually a form of Tp1.5 . Based on the data given by Craun and Smith [1970] for stilbene, this
approach yields
−1
5.397 Tp1.5
P (Tp ) = 0.0204 + 1.5  , (18.43)
Tp 5.397
where the approximation ignores the small offset of 0.0204, and P and Tp are both in units of MeV. Given
 ≈ 0.01 mg cm−2 MeV−1 and the data of Craun and Smith [1970], the values of dTp /dP for
a value of k B
stilbene are approximated by,

dTp −1.781 + 64.237 Tp + 6.77Tp
≈  , 0.005 < Tp < 15 MeV. (18.44)
dP 1 − 5.239 Tp + 26.157Ep − 1.72Tp1.5

The distortion in the pulse height spectrum from the idealized proton recoil spectrum, which is normalized
to unit height, is shown in Fig. 18.22. It is notable that the general shape of the pulse height spectrum due
solely to scintillator non-linearity is determined analytically with the use of empirical fits. The normalized
Sec. 18.3. Detectors Based on Recoil Scattering 923

luminous output, from Eq. (18.43), is described 


by
P (Tp ) ≈ c1 Tp1.5 , (18.45) 

where c1 is a constant of proportionality. Then


from Eq. (18.42) 

 
N (Tp ) 
 
N (P ) = . (18.46)
dP/dTp  
 
Because N (Tp ) is constant for Tp < E0 

c2
N (P ) =  . (18.47) 
1.5 Tp
 
From Eq. (18.45) it is seen that Tp is propor-        
tional to P 1/3 and substitution of this result into 
Eq. (18.47) yields the expected shape of the pulse
height distribution, namely Figure 18.22. Distortion of the ideal pulse height spectrum for
stilbene due to non-linear light yield. Shown is the expected pulse
c3
N (P ) = 1/3 , (18.48) height spectrum from 15-MeV neutrons.
P
where c3 is a constant of proportionality. This dependence of N (P ) on P is clearly seen in Fig. 18.22.
Statistical Fluctuations The effect of statistical fluctuations on detector energy resolution was covered in
prior chapters, mainly in Sections 6.9 and 6.10 on counting statistics and error propagation and in Section
10.5.4 for proportional counters. In general, the energy resolution of a detector is limited by the fluctuation
in charge carriers. For a scintillator, there are multiple sources of fluctuations, such as fluctuations in the
number of excited free electrons and excitons produced, the fraction of charges that decay by fluorescence, the
number of photons arriving at the light detection device, the charge carriers produced at the light detector
(photoelectrons, for instance), and the gain. These fluctuations produce a variation in the light output near
T = E0 such that dN (P )/dP assumes a Gaussian shape with mean P   E0 and a variance σP2 . This effect
softens the high energy edge by producing a sigmoid transition instead of the step function change, as shown
in Fig. 18.21(c).
Multiple Scattering Protons entering the detector may undergo scattering with carbon atoms. From
Eq. (18.4), at most only 28% of the initial proton energy can be transferred to a carbon atom with a single
scatter so that the scattered neutron has a residual energy ranging from 0.72E0 to E0 . The recoil carbon
atom also has kinetic energy, but the luminescence is low and these events are considered to add negligible
fluorescence [Swartz and Owen 1960], and hence do not contribute (appreciably) to the pulse height spectrum.
The efficiency of neutrons scattering once by carbon can be expressed by,
NC (E0 , ) ΣC
1c = = [1 − exp [−(ΣH + ΣC ) ]] . (18.49)
N0 (ΣH + ΣC )
Suppose that the energy of the carbon scattered neutrons can be defined by an average neutron energy E 1
and that these neutrons must pass through some average amount of material 1 of scintillator. If the organic
scintillator is sufficiently thick to allow at least two neutron scatters, the efficiency of proton scattering first
from carbon followed by scattering from hydrogen is
N2 (E0 , , 1) NC (E0 , ) ΣH (E 1 )   
2(ch) = = 1 − exp −[ΣH (E 1 ) + ΣC (E 1 )][ 1 ] . (18.50)
N0 N0 [ΣH (E 1 ) + ΣC (E 1 )]
924 Fast Neutron Detectors Chap. 18

The total proton scattering efficiency becomes


t = 1h + 2(ch) . (18.51)
Swartz and Owen [1960] note that the result of Eq. (18.51) is often nearly the same as if no carbon scattering
occurred, i.e., ΣC = 0. The effect on the pulse height spectrum is shown in Fig. 18.21(d). Although some
carbon scattered neutrons may exit the detector, this problem can be greatly mitigated by using detectors
that are relatively wide. Hence, carbon scattering tends to reduce the energy of some neutrons, but not
necessarily the number of proton recoils. Instead, the spectrum is shifted such that the number of counts is
slightly increased in the lower energy region, while the number of counts is slightly decreased in the energy
range between 0.72E0 to E0 . Overall the total number of counts recorded in the pulse height spectrum would
change little.
There is also the possibility of multiple proton scatters, in which two proton recoils from a single neutron
occur rapidly in succession and are recorded as a single event. Such double (n,p) scattering emphasizes the
higher energy region of the pulse height spectrum [Segel et al. 1954], an opposite effect to that of carbon
scattering. A depiction of this effect on the spectrum is shown in Fig. 18.21(d). Note that if the detector
were sufficiently thick, the total neutron energy would be deposited in the detector for each event. Because
of non-linear light yield, there would be a variance about the average luminescence per neutron, even from
a monoenergetic neutron source. Overall, these two different scattering effects tend to partially offset each
other in small detectors. In either case, the knowledge of the differential scattering cross section combined
with the knowledge of the scintillator specific light yield can be used to model the pulse height spectrum
with Monte-Carlo methods.
Edge Effects Edge effects occur as a consequence of losing recoil protons from the detector periphery. This
effect is enhanced for detectors with dimensions less than the average range of the recoil protons. A count is
still recorded for the recoil proton, but the pulse height is diminished by the amount of energy not deposited
in the detector. Intuitively, one can understand that energy loss from protons escaping the detector increases
counts in the lower energy channels while reducing events in the higher channels, as depicted in Fig. 18.21(e).
Threshold Reactions At sufficiently high neutron energies, there are threshold reactions that can be of
concern [Mösner at al. 1966; Grin et al. 1969], mainly the 12 C(n, α)9 Be and the 12 C(n, n)3α reactions with
Q-values of 5.70 MeV and 7.27 MeV, respectively. Both of these reactions release energetic heavy ions, and
consequently add to the total neutron detection efficiency [Hermsdrof et al. 1973]. However, because of non-
proportional light yield, especially for ions heavier than protons (see Chapter 13), the added luminescence
further distorts the differential pulse height spectrum. From the result of Problem 18.11, the threshold
energy for these reactions are 6.176 MeV and 7.881 MeV, respectively, as shown in Fig. 18.23.
Directional Asymmetry Thus far, it has been assumed that the light yield is relatively constant for all
proton trajectories. However, both anthracene and stilbene show directional dependence on light emission,
reportedly as much as 15% variation [Swartz and Owen 1960]. However, directional asymmetry is generally
not a problem with plastic and liquid scintillators. In the case of varied light yield with proton direction,
the overall result is an increased variance in the pulse height spectrum, further smearing and distorting the
idealized spectrum and is shown in Fig. 18.21(f).
Dependence on the Lower Level Discriminator (LLD) From Fig. 18.21(a), it becomes evident that the
pulse height spectrum ranges from channel 0 (no energy transfer) up to the total fast neutron energy E0 . If
the LLD is set to zero, then electronic noise and background radiation contaminate the spectrum.9 Hence,
it is traditional to set the LLD to discriminate neutron events from other events such as gamma ray
9 Thecondition with LLD = 0 is at times referred to as the zero bias condition, an unfortunate choice, mainly because this
condition is also used more accurately to describe radiation detectors that operate with no voltage applied.
Sec. 18.3. Detectors Based on Recoil Scattering 925



 

  !"





  



        
   

Figure 18.23. Fast neutron reaction cross sections for 12 C. Data are from
[ENDF VIII 2018].

interactions; however, such discrimination artificially reduces the


LLD = 20 keV
overall detection efficiency by eliminating low energy (n,p) recoil
events. This reduction in efficiency is non-linear, being zero for
Relative Efficiency

50 keV
proton recoils below the LLD, and also decreases as the fast
100 keV
neutron energy E0 is increased.
Suppose the LLD is set at 500 keV. Under such a condition,
only a few select events with θc  180◦ allow 500 keV neutrons
to be detected. The number of possible detectable scatter an- 500 keV
gles increases as E0 increases and produces higher efficiency for
neutron energies greater than E0 , in this example, 500 keV. The 1 MeV

overall scatter cross section for 1 H decreases with energy (see 10 1


10 2
10 3
104
Fig. 18.14), which decreases the detection efficiency even though Neutron Energy (keV)
the detectable scatter angle θc increases. Combined, these ef-
Figure 18.24. Efficiency is a function of the
fects produce a maximum in the efficiency curve as a function of LLD setting, neutron energy, and elastic scatter-
neutron energy and LLD setting, as depicted in Fig. 18.24. ing cross section.

Multiple Neutron Energies For multienergetic neutron sources, the varied emission energies will work to
further smear the features in the output spectrum. For instance, the varied energies from a PuBe source
range from hundreds of keV up to 11.5 MeV (see Fig. 5.5), with all energies being susceptible to the response
deviations described in the previous sections on ion recoils. Hence, the spectral features for proton recoils
from a multienergetic source will be a convolution of the various energies, their emission probabilities, and
combined distortion effects for each of these emission energies.
Pulse Shape Discrimination Detectors
Pulse shape discrimination (PSD) is used as a method to distinguish between different ionizing events in
a scintillation detector, already outlined in Sec. 13.3.1 under organic scintillators. The basic method takes
advantage of the different pulse output pulse shapes produced by a scintillator from heavy ions, electrons, and
926 Fast Neutron Detectors Chap. 18

Dtf Dts

number of events
pulse output

gamma rays threshold

neutrons

neutrons

gamma rays

0 time slow/fast ratio


Figure 18.25. Depiction of two different pulse shapes for a scintillator. Di-
vided into two regions, the ratios of the integrated output produce a PSD
spectrum that distinguishes between gamma-ray and heavy ion events.

gamma-rays. Gamma-ray pulses tend to be shorter with a faster decay time than those observed for heavy ion
events. Consequently, by time gating the pulse shape into two separate regions a distinct separation between
heavy ion and gamma-ray events becomes apparent. Plastic scintillators with high hydrogen-to-carbon ratios
can be used as fast neutron detectors from proton recoil events. For many scintillators, both organic and
inorganic, the pulse shapes for fast protons are much different than those for gamma-ray reactions.
Consider the depiction of scintillator output pulse shapes in Fig. 18.25(left). A time window width Δtf
is set for the fast decay component while a second time window width Δts is set for the slow decay compo-
nent. The integrated output over Δts divided by the integrated output over Δtf yields unique signatures
characteristic of gamma-rays or neutrons. The number of these pulse height ratios as a function of the
ratio value often reveals a clear distinction between gamma-ray and neutron induced pulses, as depicted
in Fig. 18.25(right). Several examples of pulse shape discrimination spectra from organic scintillators are
shown in Chapter 13.3.
Although many organic scintillators can distinguish between neutron and gamma-ray events with PSD,
there are a select few that perform better than most and are so identified in Sec. 13.3.2. Also, some inorganic
scintillators show discrimination between pulse heights for various forms of ionizing radiation. Because most
inorganic materials are more efficient at absorbing gamma rays than the organic scintillators, they are
generally not used for such purposes. However, there are some exceptions such as the use of ZnS:Ag adjacent
to a plastic waveguide.
Shown in Figs. 18.26 and 18.27 are proton recoil spectra from a 252 Cf source and an AmBe source taken
with a plastic scintillator. The pulse shapes were separated into gamma-ray and neutron events with the
pulse shape analysis technique, and then plotted as a function of pulse height digitally sorted into a sequence
of channels. Both 252 Cf and AmBe neutron sources emit a broad spectrum of energies as described in
Section 5.4. Consequently, the pulse height spectra in Figs. 18.26 and 18.27 also show continua, blurred by
the multiple effects described in Fig. 18.21, a similar result to that reported by Cester et al. [2014].

Proton Recoil Telescope


The various problems with the degradation of the energy resolution in a plastic scintillator can be reduced
if the energies of recoil protons are accurately measured. Further, if the scatter angle of the recoil proton
is known accurately, the initial neutron energy can be determined from Eq. (18.4) with A = 1. A device to
accomplish such measurements was introduced during the 1940s and is described by Johnson [1960]. The
basic device, named a proton recoil telescope, consists of a thin hydrogenous material acting as a proton
radiator with high resolution detectors positioned, in some manner, behind the radiator. This configuration
Sec. 18.3. Detectors Based on Recoil Scattering 927

 

 ! " !" #
  
    
 
 

 
 

    

  

 
                 
         

Figure 18.26. Proton recoil spectrum from 252 Cf Figure 18.27. Proton recoil spectrum from an AmBe
taken with a plastic scintillator Elgin EJ-299-33A. source taken with a plastic scintillator Elgin EJ-299-
Pulse shape discrimination was used to separate 33A. Pulse shape discrimination was used to separate
gamma-ray and neutron events. Courtesy Priyarshini gamma-ray and neutron events. Courtesy Priyarshini
Ghosh and Taylor Ochs (Kansas State). Ghosh and Taylor Ochs (Kansas State).

annular
shield radiator
neutrons
shield radiator
qr
neutrons
shadow bar
qr
detector
shield
detector
shield

(a) (b)

Figure 18.28. Proton recoil telescope spectrometers; (a) with out-of-line geometry and
(b) with annular geometry. After on Hawkes et al. [2002].

mostly mitigates the multiple problems encountered with organic scintillator spectrometers as described
in the previous sections. The purpose of the proton recoil telescope is to accurately measure the energy
of impinging fast neutrons. However, this goal also requires that the radiator be relatively thin in order
to diminish energy self-absorption and to preserve the energy of the recoiling proton. Consequently the
efficiency of the device is quite low, often below 10−4 .
There are several designs proposed for proton recoil telescopes, each intended for a specific use. In
some cases, the proton recoil telescope is used as a neutron spectrometer and the proton energy and the
scatter angle must be known accurately. Collimators can be used to ensure that only specific proton angular
trajectories are allowed to reach the particle detector [Johnson 1960]. Collimators may also be used to define
the fast neutron direction with respect to the radiator and the proton detectors located at known angles to
the radiator. For instance, Hawke et al. [2002] report on two such configurations, depicted in Fig. 18.28,
to operate as proton recoil spectrometers. The collimator is used to align the neutrons to the radiator
and the detector is offset from the neutron beam at a known angle. This out-of-line configuration reduces
direct neutron interactions in the proton detector. The annular configuration (Fig. 18.28(b)) has the added
advantage of a larger source solid angle, thereby increasing the overall detection efficiency.
928 Fast Neutron Detectors Chap. 18

To remove background interference, a thin ΔE detector can be placed in front of the proton detector
and operated in coincidence [Ryves 1976; Cazzaniga et al. 2015; Marini et al. 2017]. The thin ΔT detector
samples a small portion of energy from the proton while the main detector absorbs the remaining energy
T  . For detectors responding linearly to energy deposition, the initial neutron energy E is obtained from
Eq. (18.4) as
proportional counters
E = (ΔT + T  ) cos2 θr . (18.52)

The product of (ΔT )(T  ) gives a measure of the parti-


exit aperture
neutrons cle mass [Parkinson and Bodandsky 1965; Chaminade
et al. 1967; Homeyer 1967], and can be used to assure
platinum that the impinging particle is a proton and not another
diaphragm particle
spectrometer charged particle type. Donzella et al. [2010] describe
a proton recoil telescope with a multilayer segmented
hydrogenous
radiator, two position sensitive ΔT Si detectors, fol-
radiators platinum lowed by a CsI:Tl detector, all operated in coincidence.
apertures
The segmented radiator doubles as a position sensitive
radiator selector
wheel
organic scintillator, giving the originating location of
the (n,p) reaction. The reported energy resolution of
the fast neutrons ranged from 20% FWHM at “a few”
MeV to 2% FWHM at approximately 160 MeV, and
the device had an average efficiency of about 3 × 10−5.
Figure 18.29. A proton recoil telescope. The radiator
An advanced version, with multiple position sensitive
and the exit aperture define the acceptance solid angle of
the proton recoils. Based on Bame et al. [1957]. ΔT CMOS detectors aligned with a silicon surface bar-
rier detector is reported by Combe et al. [2018]. This
device has an in-line configuration, and the proton recoil angles are tracked between the three CMOS pixel
detectors before capturing the residual energy in the silicon surface barrier detector.
For monoenergetic neutron sources, the efficiency of the spectrometer may be the most important factor,
especially for measurements of cross sections. Early designs, still in use, have a dual chamber proportional
counter arranged between the proton radiator and a spectroscopic detector [Johnson and Trail 1956; Bame
et al. 1957; Ryves 1976; Lövestam 2006], as shown in Fig. 18.29. The geometry of these devices is an in-line
configuration. These proton recoil telescopes have several different radiators on a selector wheel that allows
the user to easily change the targets, each radiator target usually having different mass thicknesses of the
same substance. The reason for these different targets is to account for changes in (n, p) cross section as
the fast neutron energy changes [Bame et al. 1957]. The particle spectrometer can be a scintillator [Johnson
and Trail 1956; Bame et al. 1957] or semiconductor detector [Ryves 1976; Lövestam 2006]. The proportional
counters and the neutron spectrometer are operated in triple coincidence to reduce background.
Capture Gated Neutron Spectrometer
The capture gated concept is implemented with a loaded scintillator [Drake e al. 1986], most commonly an
organic scintillator loaded with 10 B, or with loaded scintillator immersed in an organic scintillator [Czirr
and Jensen 1989]. From the previous section describing the pulse height spectrum from elastic scattering
in an organic scintillator, fast neutrons produce a continuous spectrum of energies with distortions arising
from many effects. The interaction time for elastic scattering, including multiple scatters, is relatively short,
typically tens to hundreds of nanoseconds. If the neutron loses nearly all of its kinetic energy from elastic
scattering in the scintillator, the thermalized neutron continues to diffuse until it is absorbed by either a
Sec. 18.3. Detectors Based on Recoil Scattering 929

hydrogen atom (332 mb) or (less probable) with a carbon atom (3.53 mb). The 1 H(n,γ)2 H reaction releases
a 2.22 MeV gamma ray, but this gamma ray usually escapes the organic scintillator and goes undetected.
Should the neutron react with carbon, there are three possible gamma-ray emissions (1.26 MeV, 3.68 MeV,
4.95 MeV) also of high energy and most likely to escape the scintillator. If instead a small fraction of 10 B
atoms are distributed within the organic scintillator, for instance 1% loading, the chance of absorption in
the boron is over 100 times greater than in the hydrogen. Upon absorption in the boron, the 10 B(n,α)7 Li
reaction releases reaction product energy of either 2.31 MeV (94%) or 2.79 MeV (6%). In either case, these
reaction products also produce scintillation light from the detector.
Capture gated neutron spectroscopy is possible because the time required to thermalize the neutron is
much less than the time it takes for the thermalized neutron to diffuse to a 10 B location. Hence, there are two
releases of scintillation photons, first from the elastic scattering and second from the 10 B(n,α)7 Li reaction,
separated by some time period Δt, usually between 10 and 20 μs. Because it is unlikely that an epithermal
or fast neutron interacts in the 10 B, these paired scintillations occur predominantly when the initial fast
neutron has lost all of its kinetic energy. Hence, the magnitude of the first scintillation release is indicative
of the initial neutron energy and the second scintillation release indicates that the neutron did indeed lose all
(or most) of its kinetic energy. Because the Q-value of the 10 B(n,α)7 Li reaction is recognizable, it is a simple
matter of calibrating the detection system to recognize within a given Δt the two separate pulses, that the
latter emission pulse has the distinctive energy signature from the 10 B reaction. Hence, the energy of the
second pulse can also be discriminated with an energy window to ensure that it is truly from a 10 B(n,α)7 Li
reaction. If the second pulse does not appear within some set coincidence time Δt, or if the relative energy
indicates that it is not from the 10 B reaction, the former pulse is rejected. The method reduces the overall
fast neutron counting efficiency of the scintillation detector, although the quality of the energy spectrum is
improved.
Ideally, the scintillation light produced by
fast neutrons that have been thermalized in an
organic scintillator would be indicative of the
total energy deposited, regardless of the num-
ber of scatters required for thermalization. In
reality, there is an average number of scatters
needed to thermalize a neutron and also a vari-
ance about that average. For mono-energetic
neutrons, this physical result means that the
scatter angles and recoil proton energies of the
scattering events are different, although the to-
tal energy loss for fully absorbed neutrons must
still be the same for all incident neutrons. As
discussed in Sec. 13.3.1, organic scintillators re-
spond non-linearly to heavy charged particles,
especially as the specific energy loss dT /dx in-
creases. The light yield per scatter is a function Figure 18.30. Capture gated spectra from monoenergetic fast neu-
of the recoil proton energy and also the energy trons. The system consisted of a plastic scintillator annulus around
3
loss per unit distance dE/dx, thereby adding to a He gas-filled detector. Data are from Drake et al. [1986].
the variance in light yield. Consequently, the energy resolution of the neutron spectrum is much broader
than predicted by simple Gaussian statistics based on charge carrier production (see Fig. 18.30). Attempts
to mitigate the problem of non-linear light yield have been tried by using segmented detectors to compart-
mentalize the light emission, thereby allowing light yield corrections to the energy deposited [Abdurashitov
et al. 2002; Bowden et al. 2009].
930 Fast Neutron Detectors Chap. 18

Although boron-loaded plastics are a popular choice for capture-gated neutron spectroscopy [Drake et
al. 1986; Feldmann et al. 1991; Kamykowski 1992; Holm et al. 2014], many other configurations have been
reported with good results. Boron-loaded liquid scintillators have been reported with the added function of
pulse shape discrimination to eliminate gamma-ray background [Jastaniah and Sellin 2004; Flaska and Pozzi
2009]. One of the earliest implementations of capture-gated neutron spectroscopy used a plastic scintillator
annulus around a 3 He gas-filled detector [Drake et al. 1986]. Lithium can also be added to plastic or liquid
scintillators [Czirr et al. 2002; Fisher et al. 2011 ; Wilhelm et al. 2017], the advantage is a higher Q value
(4.73 MeV), a single decay branch, and no gamma-ray emissions from an excited state. A disadvantage
of using LiF is the lower neutron absorption cross section (microscopic and macroscopic) [McGregor et al.
2003]. Pulse shape discrimination methods have also been used with a Li-glass/plastic scintillator layered
structured, also operated as a capture gated detector [Czirr and Jensen 1994]. Nattress et al. [2016] describe
the use of Li-loaded glass rods arrayed in a matrix inside a plastic scintillator.
Hornyak Buttons
ZnS:Ag has a unique property of having relatively low light yield for electron interactions while being
reasonably bright for heavy ion interactions. This particular property was put to use by Hornyak in 1952
(see discussion on Zinc Sulfide in Section 13.2.2). The original Hornyak buttons were fabricated by mixing
a fine powder of ZnS:Ag with PMMA10 molding powder and curing the samples in shapes as small plugs
[Hornyak 1952]. That fact that PMMA is a non-scintillating organic helps to reduce background light from
gamma-ray events. However, in high radiation fields of mixed neutrons and gamma rays, the production of
Čerenkov emissions from the PMMA are possible (n = 1.49) and, thus, increase the background. Regardless,
Hornyak [1952] reported good efficiency for fast neutrons while still being relatively insensitive to gamma-ray
background.
At mass thicknesses of 25 mg cm−2 or greater, ZnS:Ag becomes opaque to its own light emissions. This
mass thickness is equivalent to 61 microns of pure ZnS:Ag (4.09 g cm−3 ). However, ZnS:Ag is usually
deployed as a powder mixed with a binder, which reduces the volume density of ZnS:Ag, but the opaqueness
problem remains. Because of self-absorption light losses, modern Hornyak button designs deviate from the
original design. Instead of mixing the ZnS:Ag into the PMMA, modern Hornyak buttons are usually arranged
in a bullseye pattern, with concentric alternating rings of PMMA and ZnS:Ag. Protons scatter from the
PMMA rings into the ZnS:Ag and produce light. The light subsequently emerges from the ZnS:Ag back into
the PMMA and is guided to a light sensor, usually a PMT.
Gamma-ray interactions in PMMA can produce Čerenkov radiation emissions. In low radiation environ-
ments, simple pulse height discrimination is sufficient to effectively distinguish between neutron and gamma-
ray events. However, in mixed-field high-radiation environments, the production of significant Čerenkov
radiation can require that the lower level discriminator be set at much higher channels, a setting that conse-
quently also removes neutron events and lowers neutron detection efficiency. It has been demonstrated that
PSD can improve the detection efficiency of Hornyak-style devices [Johnson et al. 2016], more than doubling
the efficiency than with pulse height discrimination alone.
PRESCILA Detector
The PRESCILA (Proton REcoil SCIntillator – Los Alamos) detector is another recoil detector based pri-
marily on proton recoils entering a ZnS:Ag scintillator layer (see Fig. 18.31). The PRESCILA detector was
developed at Los Alamos National Laboratory with the goal of producing a new REM meter of much lighter
weight than conventional polyethylene REM balls [Olsher and Seagraves 2003; Olsher et al. 2004]. The basic
device has a large central cube of Lucite that serves both as a light guide and also as a moderator to ther-
malize neutrons. The device has concentric ring style Hornyak buttons on four sides (EJ-410P in Fig. 18.32),

10 Polymethyl methacrylate with brand names such as Lucite, Plexiglas, and Acrylite.
Sec. 18.4. Semiconductor Fast Neutron Detectors 931

each recessed into borated polyethylene plates, used for fast neutron counts. On top, the detector has a
thermal-neutron detector made from a combination of 6 LiF and ZnS:Ag. The Lucite block is attached to a
PMT, and the PRESCILA wand output can be connected to a handheld survey meter (Fig. 18.31).
The response of the PRESCILA detector is reasonably flat over a wide
range of energies. The relative response per unit dose equivalent to both
H∗ (10) and NCRP-38, in which a uniform result of 1.0 for all energies is
the desired outcome, are shown in Figs. 18.33 and 18.34. The response to
neutrons is overestimated for energies below 100 keV while the response
to fast neutrons is underestimated between the energies of 100 keV and
2 MeV [Olsher et al. 2004]. The overall response was designed to pro-
vide a relatively uniform dose equivalent. Comparatively, the response
from the Hankins rem ball and the Andersson-Braun cylinder seem to
be flatter over these same energy regions. At energies between 2 MeV
to 20 MeV, the response from the PRESCILA becomes relatively flat,
while the responses from the Hankins rem ball and the Andersson-Braun
cylinder both, almost identically, decrease as energy is increased above 7
Figure 18.31. A commercial pro-
MeV. Finally, the PRESCILA detector is considerably smaller and weighs ton recoil dosimeter. The black cu-
only 4.5 lbs (2 kg), which is much less than the rem ball or cylinder. For bic object is a PRESCILA detector
handheld field instruments, size and weight are important considerations. (see description in text).

Gas-Filled Scintillation Detectors


Recall from Sec. 13.4 that several gases were discovered to scintillate, often in the UV region.11 Of these
gases, He is the best candidate for use in a gas recoil scintillation detector, mainly because of its lower
atomic number compared to those of the other noble gases so that more energy is transferred to a recoil
atom from a neutron scattering event. For 3 He gas, there is also the possibility of producing energetic ions
from the (n,p) reaction that can also cause the gas to fluoresce. The use of 4 He gas as a recoil scintillator,
rather than as a proportional counter, mitigates problems associated with charge collection and avalanche
production [Chandra et al. 2012]. Further, the response speed is faster than in a proportional counter and
the scintillation mechanism allows the use of pulse shape discrimination methods. The kinematics of (n,α)
scattering are the same as described for proportional counters; hence the maximum energy transfer per
neutron scatter is only 64%. The recoil 4 He ions fluoresce the gas, and photomultiplier tubes (PMT) [Jebali
et al. 2015] or compact silicon photomultipliers (SiPM) can be used to measure the light yield [Arktis 2017].
A pressurized tube filled with 4 He gas is attached to a light collection device, and because charge carrier
collection is not required and charge mobility is not an issue, these chambers can be pressurized, in some
cases up to 150 atm [Kelley et al. 2015]. The high pressure reduces the recoil 4 He ion range and, consequently,
also the wall effect so that the overall efficiency for the neutron interactions is increased.

18.4 Semiconductor Fast Neutron Detectors


The use of a hydrogenous radiator, such a polyethylene, attached to a semiconductor diode has been explored
as a compact fast neutron detector and as a beam port monitor [Klann and McGregor 2000, 2002; Klann et
al. 2001, 2002; De Lurgio et al. 2003]. These detectors rely on the recoil proton entering a Schottky or pn
junction diode. The energy recorded is the proton recoil energy minus the energy self-absorption losses as
the proton traverses the radiator. The maximum range of the proton limits the useful radiator thickness and,
consequently, also determines the efficiency as a function of neutron energy. The maximum range of 14-MeV

11 Theonly noble gas that appears not to effectively scintillate is neon [Northrop and Gursky 1958], although liquid neon does
have use as a scintillator [Nikkel et al. 2008].
932 Fast Neutron Detectors Chap. 18

Figure 18.33. The energy response functions per unit dose for
the PRESCILA detector compared to a Hankins rem ball and an
Andersson-Braun cylinder. Data are from Olsher et al. [2004].

Figure 18.32. Exploded view of a PRESCILA Detec-


tor. Courtesy Ludlum Measurements, Inc.

Figure 18.34. Detail of the fast neutron energy response functions


per unit dose for the PRESCILA detector compared to a Hankins
rem ball and an Andersson-Braun cylinder. Data are from Olsher et
al. [2004].

protons in high density polyethylene is approximately 2.2 mm, with lower energies having smaller ranges.
The neutron interaction efficiency is combined with the recoil energy and solid angle, the escape probability
of the recoil proton, and the LLD setting to determine the efficiency as a function of energy [Klann and
McGregor 2000]. Models indicate that 0.11% detection efficiency is possible for 14-MeV neutrons with a 2.2
mm HDPE attached to a semiconductor diode. In general, the fast neutron detection efficiency is relatively
low for these detectors, but their compactness and low power requirement are advantageous under special
conditions [De Lurgio et al. 2003].
Sec. 18.5. Detectors Based on Absorption Reactions 933




 



!









    

   

Figure 18.35. Absorption cross sections for 3 He, 6 Li, and 10 B in the fast neutron
region. Data are from [ENDFPLOT 2017].

There are several direct interactions that can also induce pulses from the semiconductor detector. For
instance, Si is a frequent choice for a particle detector, mainly because of its relatively low absorption
coefficient for gamma rays. However, fast neutrons can interact in Si and release ionizing particles. For
instance, the (n,p) and (n,α) reactions can produce energetic particles directly in the semiconductor, ions
which do not suffer self-absorption. Although produced by neutrons, these events are considered part of the
background as are possible gamma-ray interactions [Dearnaley and Northrop 1966]. One method used to
reduce background is a compensated diode in which one section of the diode is covered with a hydrogenous
radiator while the remaining area, of equal size, remains bare. The hydrogenous side records both proton
recoils and background, while the bare side records background, and, thus, can be subtracted.

18.5 Detectors Based on Absorption Reactions


As described in Chapter 17, there are many thermal-neutron detectors based on absorption reactions. How-
ever, there are only a few isotopes with high thermal-neutron absorption cross sections that produce spon-
taneous ionizing reaction products. These same materials can be used for epithermal and fast neutron
detection, although the absorption cross sections are reduced. The two most popular absorption reactions
for fast neutron detection are the 3 He(n,p)3 H and the 6 Li(n,t)4 He reactions, whose cross section is shown in
Fig. 18.35.
3
18.5.1 He Detectors
3
He proportional counters are a popular choice for thermal-neutron detection; however, they are also
used for fast-neutron detection with combined effects from recoil scattering, fast-neutron absorption,
and thermal-neutron absorption. A few possible event trajectories are depicted in Fig. 18.36. As
with thermal-neutron detection, the fast neutrons, with energy E, may become moderated outside of
the detector, and then absorbed in the detector with negligible kinetic energy transferred to the reac-
934 Fast Neutron Detectors Chap. 18

tion products. Such a trajectory, depicted in track 4, results in the deposition of the 3 He(n,p)3 H Q-
value of 0.764 MeV in the gas. Alternatively, the neutron may be fully moderated in the detector
(unlikely) and then be absorbed in the gas, as depicted
4
in track 1, so that a total energy of E + 0.764 MeV 2 Cd sheath
n (optional)
is absorbed in the gas. Although the absorption cross n 1
3
section for He is small for fast neutrons, there is also p t
He-3
a small possibility that the neutron becomes fully ab- p
sorbed with the reaction products producing an energy t
t He-3
deposition of En + 0.764. Such an event is depicted as He-3 p
track 2 in Fig. 18.12. Finally, a recoil scatter may occur 3
n
and the scattered neutron leaves the system, as shown
by track 3, so that a continuous distribution of energies Figure 18.36. Neutron interaction possibilities for a 3 He
up to 0.75E is deposited, the maximum recoil energy gas detector.
as given by Eq. (18.4) (see Example 18.3). The idealized shape of this continuum component is given by
Eq. (18.28). When all of these possible outcomes are combined, the resulting pulse height spectrum of the
energy deposited in the gas has fast effects superimposed onto the traditional thermal-neutron response as
shown in Fig. 18.37.

Example 18.3: Determine the energies of the spectral features produced by monoenergetic 6 MeV neutrons
interacting in a 3 He detector.

Solution:
1. There is a thermal-neutron peak at 0.764 MeV from slow neutrons interacting directly with the 3 He
by the 3 He(n,p)3 H reaction.
2. The elastic scatter reaction results in an endpoint energy, given by Eq. (18.4), of

4A (4)(3)
T = E= (6) MeV = 0.75(6 MeV) = 4.5 MeV.
(A + 1)2 42

3. The full energy peak is at an energy equal to the total kinetic energy added to the Q value, namely,
6.764 MeV.

Typically 3 He gas-filled neutron detectors are designed as cylindrical proportional counters [Shalev and
Cuttler 1973], mainly because of the many advantages already described in Chapter 10. Recall that the
electronic pulse is formed primarily from ion motion, and that after the Townsend avalanche has progressed,
over 50% of the signal is generated as the ion cloud travels a distance of only a few microns from the anode
wire. Consequently, a spectrum can be formed, albeit a relatively low resolution one. To improve the energy
absorption efficiency of the recoil He ions, aimed at decreasing the wall effect, a heavy gas with greater
stopping power can be added. Candidates include Ar, Kr, and Xe, each having a lower ionization potential
than He. However, all of these gases also have lower electron and ion mobilities than He. The use of long
shaping times several microseconds long are encouraged for best results [Shalev and Cuttler 1973]. The
addition of CO2 or CH4 can help increase the average charge carrier velocities [Shalev and Cuttler 1973;
Owen et al. 1981]. Regardless, the pulse height spectrum becomes more complicated from recoils with these
added fill gases. There have been reports on the rejection of elastic scatter events through pulse height
discrimination [Sayres and Coppola 1964].
Sec. 18.5. Detectors Based on Absorption Reactions 935

0.764 MeV

thermal/

Counts per Channel


epithermal peak

En + 0.764 MeV
full energy
elastic scatter peak
recoil continuum
0.75 En

Channel Number (Energy)

Figure 18.37. The main spectral features resulting from fast neutrons inter-
acting in a 3 He detector.

Other designs include the gridded ion chamber, configured as a cylindrical design with a concentric grid12
surrounding the central anode wire [Franz et al. 1977; Sailor and Prussin 1980; Owen et al. 1981]. Recall
from Sec. 9.5.5 that gridded ion chambers rely almost entirely on electron motion and can have better energy
resolution than proportional counters. The lower electric fields used to operate gridded ion chambers reduce
the electron velocities, and, consequently, increases dead time. The counting gas is commonly a mixture
of different gases, including 3 He, Ar, and CH4 [Owen et al. 1981). The results of Franz et al. [1977] and
Owen et al. [1981] demonstrate the relatively good energy resolution that is achievable. An example neutron
spectrum from a gridded ion chamber is shown in Fig. 18.38.
Although the recoil spectrum is complicated by the addition of other gases than 3 He, Owen et al. [1981]
discuss unfolding methods that can be used to produce a neutron energy pulse height spectrum. Franz et
al. [1977] list many difficulties encountered with these detectors, including distortions from the wall effect,
proton recoil contributions (from the CH4 in the gas mixture), interaction location dependent rise times,
gamma-ray background, and microphonics. The thermal-neutron signal can be suppressed by inserting the
3
He detector into filter composed of cadmium and boron [Franz et al. 1977]. Such methods diminish the
elastic scatter and thermal-neutron portion of the spectrum while preserving the full energy peak of the fast
neutrons (Q + E). With the techniques outlined in Franz et al. [1977], reasonably high energy resolution of
complex fast neutron spectra can be achieved.
6
18.5.2 LiI:Eu Scintillators
Scintillators can also be used as direct conversion detectors if at least one element in the scintillator compound
produces spontaneous reaction products upon the absorption of a fast neutron. A drawback is that the most
commonly used neutron absorption solid state materials, 6 Li and 10 B, have very reduced interaction cross
sections in the fast neutron region.
Discussed in Chapters 13 and 17, and also previously in this chapter for moderated devices, the scintillator
6
LiI:Eu has also been applied directly for fast neutron measurements. The concept is similar to the use of
3
He as a fast neutron detector. Fast neutrons that directly interact 6 Li(n,t)4 He yield reaction products with
a total Q-value of 4.78 MeV. The kinetic energy of the reaction is added to Q-value to produce a full energy

12 The reference Shalev and Cuttler [1973] is the often quoted source of the cylindrical gridded 3 He chamber design. However,
there is no mention of a grid in this paper, Frisch is not referenced, and the authors clearly refer to the device as a proportional
counter and not a gridded ion chamber.
936 Fast Neutron Detectors Chap. 18








  

 
 
 

 
 


  



 


       

   

Figure 18.38. Delayed neutron spectrum from 137 I measured with a 3 He


gas-filled gridded ion chamber. Data are extracted from [Franz et al. 1977].

of the reaction at E + Q. Murray [1958] and Johnson et al. [1969] describe competing fast neutron reactions
that can complicate the spectrum. The spectrum is further confused by the intrinsic non-linear response
of 6 LiI:Eu to fast neutrons at room temperature. Consequently, the energy resolution for fast neutrons in
6
LiI:Eu is relatively poor. Murray [1958] and Johnson et al. [1969] found that cooling the 6 LiI:Eu crystal to
cryogenic temperatures, near that of liquid nitrogen, greatly improved both the linearity and resolution of
the detector. Example pulse height spectra of fast neutrons (5.3 MeV) at different temperatures are shown
in Fig. 18.39.
6
18.5.3 Li Sandwich
Thermal-neutron detection with 6 Li foils or 6 LiF lay-
ers between detection media has been described thor- neutrons
oughly in Sec. 17.3.2. This “sandwich” structure, pos-
sibly first explored by Love and Murray [1961] is de- semiconductor

picted in Fig. 18.40. It can also be used for fast neutron


detection, although there are some notable differences
in performance. Analysis of the detection efficiency for LiF
thermal neutrons is simplified by assuming that the re- thermal
response
action particle trajectories are emitted in opposite di- semiconductor
rections. However, for neutron energies above thermal
(0.0259 eV), their kinetic energy must be added to the
Figure 18.40. The LiF sandwich depicting possible reac-
Q-value of the 6 Li(n,t)4 He reaction (see Problem 13). tion product trajectories for fast neutron interactions.
For slow neutrons, this added energy has little effect on
the reaction product trajectories, so that the simplifying approximation that the reaction products are gener-
ally emitted in opposite directions can still be used. However, for epithermal and fast neutrons the emission
angle between reaction products is less than 180◦ . The emission angle decreases as E increases and the
reaction products are emitted increasingly in the general direction of the original incident neutron.
Sec. 18.5. Detectors Based on Absorption Reactions 937

Figure 18.39. 6 LiI:Eu scintillator pulse height spectra at different temper-


atures for 5.3 MeV neutrons. The energy resolution of the full energy peak
improves as the temperature is lowered, with FWHM of 18% (RT), 15% (231
K), 12% (181 K), and 10% (131 K). Data are extracted from [Murray 1958].

Background can be significantly discriminated from thermal-neutron detection by operating the two
detectors in coincidence, but this operation comes at the expense of detection efficiency [McGregor et al.
2003]. Unfortunately, it can be an inefficient detection method for fast neutrons, mainly because the chance
of coincidence decreases as the neutron energy increases. Because of energy self-absorption as the reaction
products pass through the LiF foil, the total energy deposited in the detector has a broad spectrum instead
of a single energy peak. This energy loss effect can be reduced by using LiF foils that are much thinner
than the combined reaction product ranges, although this approach also reduces the efficiency [Dearnaley
and Northrop 1966], which is further diminished by the reduced absorption cross section at high neutron
energies. Detailed responses and efficiencies for a 6 Li sandwich structure are described by Rydin [1968].
Bishop [1968] and Silk [1968] report on results from a 6 LiF sandwich. Most of the calibrations were
conducted with thermal neutrons, although both works report results from fast neutrons. In both cases,
a thin LiF radiator produced higher resolution results, and produced rough neutron spectra from nuclear
reactors. Rickard [1973] describes methods to improve the fast neutron energy resolution, using either
a summing technique or isolating and measuring only the triton emission. Unfolding methods have also
been employed to improve resolution [Seghour and Sens 1999]. The drawback to this particular use of
semiconductors in a reactor environment is the rapid destruction of the semiconductor detector [Gersch et
al. 2002].
Although gamma-ray interactions in low Z semiconductors (Si, SiC) are generally small, neutron events
may not be easily discriminated from other possible radiations and interactions. Sources of background can
also arise from direct interactions in the semiconductor. For instance, direct (n,p) reactions in Si produce
energetic reaction products. Because these protons are released directly in the semiconductor, they do not
suffer self-absorption effects. Consequently, the protons can produce pulses similar in magnitude to those
produced by the 6 Li(n,t)3 H reaction [Rydin 1968]. This damage effect in silicon has been proposed as a
possible fast-neutron dosimeter [Kramer 1966].
938 Fast Neutron Detectors Chap. 18

18.5.4 The Grey Detector


Closely related to the Hankins rem meter (or Bonner spheres) is the so-called “grey” detector [Pönitz 1968].
Recall that the Hankins rem meter is operated by moderating fast neutrons in a hydrogenous ball of material
that, upon thermalization, could migrate to an internal thermal-neutron detector. The grey detector operates
in a similar fashion, except that the neutron detector is removed. Instead, the thermalized neutron may
be absorbed in the hydrogenous material, promptly emitting a 2.2-MeV gamma ray. A NaI:Tl detector
placed adjacent to the moderator is used to detect these gamma rays, thereby yielding a measure of the
neutron interactions. Pönitz [1968] assumes that (1) the moderating ball is of adequate size to moderate
and absorb the neutrons with negligible leakage and (2) gamma rays escape the moderating material with
no absorption. These two assumptions are valid for neutron energies ranging from thermal to 2 MeV for a
moderator sphere (water or paraffin) between 20 and 25 cm diameter [Pönitz 1968]. The efficiency response
for neutrons with energies from thermal to 2 MeV neutrons is relatively flat. However, for neutrons with
higher energies, knowledge of the neutron leakage becomes increasingly important in order to determine the
detector efficiency [Poenitz 1969].

18.5.5 Cryogenic Detectors


A low temperature solution to neutron spectroscopy was investigated by de Marcillac et al. [1993] and
Richardson et al. [1998]. These devices are called both bolometers or microcalorimeters interchangeably,
although there is a difference in function between the two (see Chapter 19). The difference between the
two devices is that a bolometer measures the amount of radiation incident upon the device (similar to a
current mode device), whereas a calorimeter measures the energy of individual interactions in the device
(similar to a pulse mode spectrometer) [Kraus 1996]. In a bolometer the radiation absorber is attached
to a thermally sensitive electronic component, typically a thermistor.13 Both of these cryogenic detectors
measure the thermal energy deposited in a low temperature (milli-Kelvin or mK) radiation absorber. The
increase in heat in the absorber is converted into an electronic pulse, yielding a measure of the heat change
and, thus, the energy deposited.
Bolometers for radiation detection are cryogenically cooled through a heat sink that returns the absorber
and thermistor to the pre-irradiation equilibrium condition. A voltage is applied to the thermistor to produce
a steady-state current. When radiation deposits energy in the absorber, the thermistor temperature increases,
causing a change in current flow. This change can be measured as a current or voltage pulse, either being
indicative of energy absorbed.
A microcalorimeter can be fashioned by attaching an absorber to a superconducting film. Below a specific
transition temperature, the resistance of the superconductor is zero. If the temperature is set slightly below
that temperature, then heat added to the system moves the superconductor above the transition temperature
so it no longer has zero resistance. Consequently, current flow through the superconductor material now
produces a voltage, which gives a measure of the energy deposited in the absorber. This type of calorimeter
is called a transition edge superconducting (TES) spectrometer.
Bolometers and microcalorimeters have been demonstrated as functional neutron spectrometers [de Mar-
cillac et al. 1993; Silver et al. 2002]. These devices work, usually, by attaching a material that incorporates
either 6 Li or 10 B to a thermally sensitive electronic device. For either coating, the neutron reaction results
in energy deposition of the Q-value plus the neutron kinetic energy. The work of de Marcillac et al. [1993]
describes the use of a 2-g sample of 6 LiF operated below 100 mK and describes the difference in response for
different ionizing particles. Measured results indicated that the (n,α) reaction produced counts in a lower
energy channel than anticipated from calibrations with monoenergetic alpha particles.

13 A type of resistor in which the resistance is a function of the temperature.


Sec. 18.5. Detectors Based on Absorption Reactions 939

Neutron sensitive bolometers or microcalorimeters use energetic neutron reactions to deposit energy in
the absorber, most commonly the 6 Li(n,t)4 He and the 10 B(n,α)7 Li reactions. While the work by de Marcillac
et al. [1993] focused on the use of LiF as the absorber, Richardson et al. [1998] investigated the use 6 LiPb as
an absorber for a neutron bolometer. In both studies, thermal neutrons were the radiation of interest. Energy
resolution as low as 16 keV FWHM was observed for a 2-g sample of LiF operated at 10 K [de Marcillac et
al. 1993; Silver et al. 2002] also report on an optimization study with enriched 6 LiF as a thermal-neutron
detector, the largest sample being 1 cm3 . The best results were obtained from the smaller sample, 4 × 4 × 2
mm3 and produced an energy resolution of 39 keV FWHM with pulses having a 80 μs rise time and 3.1 ms
decay time.
Niedermayr et al. [2004] investigated the 10 B(n,α)7 Li reaction with a TiB2 calorimeter, and also the
6
Li(n,t)4 He reaction with 6 LiF bolometers [Niedermayr et al. 2007; Hau et al. 2006]. Although the purpose
of exploring TiB2 as a TES microcalorimeter was to produce a fast neutron spectrometer, Niedermayr et al.
[2004] describe results only for thermal-neutron reactions and report 10.5 keV FWHM for the excited state
(2.31 MeV) and 5.5 keV FWHM for the ground state (2.792 MeV).
Fast neutron spectroscopy was explored by Hau et al. [2006] with 6 LiF samples, in which fast neutrons
of energy E deposit total energy of Etotal = E + Q in the absorber. Energy resolution of 55 keV FWHM
was reported for thermal neutrons. Spectra were also reported for a 252 Cf source. There was a clear spectral
separation between neutron absorption events and the other events resulting from either elastic scattering
or gamma-ray interactions. A single elastic recoil from 6 Li can, at most, deposit only 0.49E. The residual
energy can be recovered if the scattered neutron is subsequently absorbed. Otherwise, a substantial gap
appears between the elastic scatter spectrum and the absorption spectrum. A similar situation occurs
for gamma-rays, mainly because they most likely interact in the LiF crystal through Compton scattering,
thereby also depositing only a fraction of their energy. Also, Hau et al. [2006] note that certain features
in the absorption pulse height spectrum reflect the energy dependence of the 6 Li(n,t)4 He energy-dependent
microscopic absorption cross section. Niedermayr et al. [2007] expand on the 6 Li fast neutron detection by
describing a simple unfolding method to recover the actual energy distribution from the neutron source,
which can be quite different from the elastic scattering or absorption spectrum.
Merlo et al. [2015] describe a TES microcalorimeter made of a Nb strip coated with 450 nm of natural
boron. The difficulty with this structure is similar to that of a thin neutron absorbing detector [McGregor
and Shultis 2004], namely, the absorber is too thin to (efficiently) absorb the total Q-value energy of the
(n,α) reaction or that of a fast neutron. Consequently, the device may operate as a neutron counter, but
not as a neutron spectrometer. Shishido et al. [2017] expand on this same concept by applying 10 B to
a serpentine Nb superconducting electrode. Instead of using the TES method, Shishido et al. [2017] use
another superconducting phenomenon, in which energy deposited in the superconductor causes a change in
the magnetic inductance by a decrease in the Cooper pair density.14 This device, called a microwave kinetic
inductance detector (MKID), allows the position of interacting neutrons to be determined in one dimension
along the serpentine pattern, reportedly with 1.3 mm spatial resolution.

18.5.6 Foil Activation Methods


One of the earliest methods for determining the energy dependence of the neutron field was the placement of
different foils in the neutron field, and from the activity produced in the irradiated foils, the energy spectrum
of the neutrons could be inferred. One of the earliest publications on the subject [McElroy et al. 1967] used
a hand analysis to analyze the foil data. Because each foil material has cross sections with different energy
dependence, the activation of each foil changes as the neutron spectrum changes. In Sec. 17.8 a detailed
description of how a gold foil, bare and cadmium covered, can be used to determine characteristics of a

14 Cooper pairs are the fundamental conduction mechanism in superconductors. See Cooper [1956] and also Ogg [1946].
940 Fast Neutron Detectors Chap. 18

typical neutron spectrum from a thermal reactor. In this section it is seen that the use of multiple foils can
be used to determine a neutron energy spectrum in a way that is very similar to that used by the Bonner
spheres. In fact, unfolding Bonner sphere measurements is exactly the same as unfolding foil activities and
the same unfolding algorithms have been used for both.
The term foil as used here can be in various forms: powder, wires, or actual metallic foils although they
are “small” to reduce self-absorption effects and to give good spatial resolution. For fluxes that have high
energy neutrons, materials that have threshold cross sections are attractive. Typically ten or so different
foils are used and activities are measured when the foils are irradiated, both when bare and when covered
by some slow neutron filter material (typically, cadmium or gold). There appears to be no best set of foils
to use in all situations. Some widely used foil reactions are listed in Table 18.2.

18.5.7 The Foil Inversion Problem


With the method discussed in Sec. 17.8.2, the saturation activity can be determined by counting the radiation
emitted by a particular radioisotope produced by the neutron irradiation of a foil. Usually a gamma ray of
a well-defined energy is counted, although beta-particle counting is also sometimes used. Division by the
number of activation target atoms that are in the foil gives the specific saturated activity Ai per target atom
at infinite dilution (so the burnup of the activation product can be ignored) for the ith activation reaction.
Further, this specific activity is corrected for self-shielding and flux depression. This activity is given by the
Fredholm integral equation  ∞
Ai = Ri (E)φ(E) dE i = 1, . . . , N. (18.53)
0

Here φ(E) is the energy dependent flux at the point of interest and the response function is

Ri (E) = σi (E) exp[−Nc xc σc (E)], (18.54)

where σi (E) is the microscopic activation cross section for the ith reaction. The exponential term accounts
for a cover material, such as cadmium, placed around the foil to suppress activation by thermal or epithermal
neutrons. The cover has an atom density of Nc , thickness xc , and absorption cross section σc (E). For a bare
foil xc = 0 and the exponential term in Eq. (18.54) is absent.
Estimation of the Energy-Dependent Flux
In principle, any method used to solve the Bonner sphere problem of Eqs. (18.9) can be used to invert the foil
activation problem. A general overview is provided by Cross and Ing [1987]. Here the basis of the SAND-II
code [McElroy et al. 1969] is reviewed because it was the first code upon which many subsequent codes with
minor algorithmic changes and additional features, such as enhanced error analysis, are based. To convert
Eqs. (18.53) a contiguous energy grid Ej , j = 1, . . . , M is defined such that φ(E) = 0 if E < E1 or E > EM .
The grid spacing is Δj = Ej+1 − Ej . In SAND-II, 620 energy intervals are used covering the range 10−10 to
18 MeV (45 intervals per decade up to 1 MeV and 170 intervals between 1 and 18 MeV).
Equations (18.53) can be written as

M 
 Ej+1 
M
Ai = Ri (E)φ(E) dE ≡ Aij i = 1, . . . , N. (18.55)
j=1 Ej j=1

The solution procedure begins by assuming an initial flux guess φ0j , Ej ≤ Ej+1 and then this flux is refined
iteratively φkj , k = 1, 2, . . . , K by making the calculated partial activities Akij , which depend on φkj , to agree
with the measured activities Ai to within some specified tolerance. To calculate the activity, it is first assumed
Sec. 18.5. Detectors Based on Absorption Reactions 941

Table 18.2. Some activation foils used for thermal- and fast-neutron measurements. Most foils
are irradiated with Cd, Au, or 10 B covers to suppress contributions from thermal and epithermal
neutrons.

Nat. Threshold γ-rays (MeV)


Element Reaction Half-Life
abundance energy (MeV) [yield %]

27 Al(n,p)27 Mg 0.8437 [71.8]


Al 100 1.896 9.45 min
1.0144 [28.0]
27 Al(n,α)24 Na 1.369 [100]
100 3.250 14.95 h
2.754 [99.9]

Au 197 Au(n,2n)196 Au 100 8.114 0.3557 [23.07] 6.167 d


197 Au(n,γ)198 Au 100 0 0.41180 [95.51] 2.6952 d

Cu 63 Cu(n,2n)62 Cu 69.1 11.038 0.511 [195.6] 9.74 min


65 Cu(n,2n)64 Cu 30.83 10.064 0.511 [35.7] 12.701 h

63 Cu(n,α)60 Co 1.173 [99.86]


69.17 0 5.271 y
1.332 [99.98]
63 Cu(n,γ)64 Cu 69.17 0 0.511 [35.7] 12.701 h

59 Co(n,γ)60 Co 1173 [99.86]


Co 69.1 0 5.271 y
1332 [99.98]
Fe 56 Fe(n,p)56 Mn 91.7 2.966 0.8469 [99.87] 2.578 h
54 Fe(n,p)54 Mn 5.85 0 0.8348 [99.97] 312.1 d

In 115 In(n,n )115m In 95.71 0.336 0.3363 [46.71] 4.485 h

Mg 24 Mg(n,p)24 Na 78.99 4.932 1.368 [99.99] 14.95 h

Mn 55 Mn(n,γ)56 Mn 100 0 0.8468 [98.87] 2.578 h

Ni 58 Ni(n,2n)57 Ni 68.08 12.478 1.378 [77.9] 36.1 h


58 Ni(n,p)58 Co 68.08 0 0.8107 [99.44] 70.88 d

Th 232 Th(n,f)140 La 99.27 − 1.5962 [95.49] 1.678 d

Ti 47 Ti(n,p)47 Sc 7.44 0 0.1594 [68.0] 3.349 d

46 Ti(n,p)46 Sc 0.8896 [99.98]


8.25 1.619 83.81 d
1.211 [99.98]
0.9835 [100.0]
48 Ti(n,p)48 Sc 73.72 3.274 1.0375 [97.5] 43.7 h
1.3121 [100.0]

U 238 U(n,f)140 La 99.27 − 1.5962 [95.5] 1.678 d


238 U(n,f)140 Ba 99.27 0 0.5373 [23.5] 12.75 d

Zr 90 Zr(n,2n)89 Zr 51.45 12.102 0.9091 [99.04] 3.27 d


942 Fast Neutron Detectors Chap. 18

the cross sections are constant over an energy interval, i.e.,


 Ej+1
1
σ ij  σi (E) dE. (18.56)
Δj Ej

Likewise the cover cross section is a constant σ c over each energy interval. Thus for the k iteration

Akij = σ ij exp[−Nc xc σ cj ]φkj Δj = Rij φkj Δj , (18.57)

from which the calculated activity Ai for the ith reaction is found from Eq. (18.55).
To update the flux profile, two parameters are used: an activity weighting term Wij = Akij /Akj and a
so-called activity-weighted correction term
%N
Wijk ln(Ai /Aki )
Cjk = i=1%N . (18.58)
k
i=1 Wij

The next estimate of the flux is then computed as

φk+1
j = φkj exp(Cjk ). (18.59)

This iterative procedure is continued until the standard deviations of the ratios of measured to calculated
activities is less than some specified value. There is also a foil discard test such that if the measured activity
of a particular reaction deviates more than some specified number of standard deviations from the calculated
value that foil is removed and another solution without that foil is obtained.
The background and methodology of the SAND-II code has been extensively studied (see references cited
by McElroy et al. [1969]). There are many other unfolding methods and codes available, some of which are
reviewed by Moghari [1979].

18.6 Summary
In this chapter many different types of fast neutron detectors have been briefly described. The detection
of fast neutrons is accomplished by using one of the following three techniques. (1) The fast neutrons are
first moderated to lower energies and those that become thermalized are detected using thermal neutron
detectors. Bonner spheres and rem balls are examples of fast neutron detectors based on the moderation
principle. (2) Charged recoil atoms produced by fast neutron scattering can be measured in charged particle
detectors. This technique is the basis for many types of recoil spectrometers. (3) Finally, fast neutrons
can often produce nuclear reactions not possible with thermal neutrons and products of these fast neutron
interactions can often be measured and the fast neutron flux can be inferred. Foil activation methods typify
the use of this method to distinguish neutrons with a wide range of energies.
In almost all of these detectors indirect information about the energy dependence of the neutron field is
obtained and, hence, they can also be used as neutron energy spectrometers and not just detectors. However,
their use as energy spectrometers is not as straightforward as, say, with gamma-ray spectrometers where full
energy peaks in the output pulse height spectrum immediately give the energies of incident monoenergetic
gamma rays. The output spectrum from neutron spectrometers, by contrast, is not easy to interpret for two
main reasons. First, most neutron fields have a continuum of neutron energies without any superimposed
monoenergetic peaks. Second, the output pulse height spectrum from a fast neutron spectrometer often bears
little resemblance to the neutron spectrum. Consequently, the output must be post-processed or unfolded to
recover energy information about the incident neutrons. In fact, the output from any radiation spectrometer
needs to be unfolded to recover all details of the energy dependence of the incident radiation. Although a
Problems 943

few brief discussions are given in this chapter about the unfolding or deconvolution of the output from fast
neutron devices, the general topic of unfolding is worthy of several chapters, or even a book, to be treated
thoroughly.

PROBLEMS
1. For A = 1, show that Eq. (18.2) implies that θc = 2θs .
2. Determine the thermal neutron absorption length for a 3 He gas-filled detector pressurized to 4 atm. If
the detector is 1 inch in diameter (2.54 cm), what is the maximum attenuation for a beam of neutrons
intersecting perpendicularly the tube cross section?

3. You have a 10 BF3 detector built from a 25 mm diameter (I.D.) Al tube, backfilled with 0.2 atm of 10 BF3
and 2 atm of Ar gas. If a 0.5 cm diameter thermal neutron (2200 m s−1 ) beam intersects through the
detector mid-section, what is the expected intrinsic thermal neutron detection efficiency?
4. Given a a thermal neutron beam (0.025 eV) intersecting a 10-mm-thick
5. sample of CLYC:Ce, determine the intrinsic thermal neutron detection efficiency of the CLYC:Ce sample.
If the natural Li is replaced with 96% enriched 6 Li, what is the new thermal-neutron detection efficiency?

6. Plot ωc versus the corresponding ωs for A = 1, 2, 4, 10, 50, 100, and 200. What does this graph reveal
about the center of mass and laboratory coordinate systems as A becomes large?

7. The speed of the K-shell electrons in 4 He, as given by the Bohr model [Shultis and Faw 2016] as
vK = e2 /(o h). Compare this speed to that of a 4-MeV recoil 4 He atom. At this recoil speed, the
shake-off effect has removed almost all of the electrons from the helium, so that a 4-MeV 4 He beam in
gas has about an average charge of +1.99e per atom [Evans 1955].
8. Derive Eq. (18.24) from Eq. (18.23).
9. Derive Eq. (18.27).

10. Consider a general binary nuclear reaction X(x,y)Y and use the conservation of energy and momentum
constraints, as used in Chapter 4, to show
< <
 mx my Ex mx my Ex mY − mx mY Q
Ey = ωy ± ω2 + Ex + ,
(my + mY )2 (my + mY )2 y (my + mY ) (my + mY )

where the Q-value is


Q = (mx + mX − my − mY )c2 .

11. From the previous problem for exoergic reactions Q < 0, show the kinematic threshold for this reaction
is  
m y + mY mx
Exth = − Q 1+ Q.
my + mY − mx mX

12. Find the Q-values and threshold energies for the reactions (a) 12 C(n, α)9 Be and (b) 12 C(n, n)3α. The
threshold energies can be calculated from Eq. (4.46) and from the formula developed in the previous
problem.
944 Fast Neutron Detectors Chap. 18

13. From the result of Problem 18-9 show that for exoergic reactions (Q > 0) as Ex → 0
mY my
Ey = Q and EY = Q,
my + mY my + mY

so that
Q = Ey + EY .

14. The energetics of the 6 Li(n,t)4 He reaction are given in Sec. 17.2.3 for a thermal neutron. If the same
reaction is caused by a 1-MeV neutron, what are the kinetic energies of the reaction products? As the
energy of the neutron increases, how does the angle between the reaction products change?

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Chapter 19

Luminescent, Film, and


Cryogenic Detectors
The crystals were swallowed by the patients, recovered one or two days later, and the
accumulated dosage in roentgens was measured by matching the thermoluminescence
intensity with that produced in the crystals by a known roentgen dosage.
Farrington Daniels

19.1 Luminescent Dosimeters


A luminescent dosimeter is a type of phosphorescent detector that can store energy information for extended
periods of time. This passive readout detector has the property of storing electronic charges in deep traps
that are later depopulated with an intentional and controlled sampling method. Hence, a luminescent
detector is a type of integrating dosimeter. Typically, the device can be reused after the reading of the
accumulated dose is complete. Luminescent dosimeters are popular for radiation dosimetry because of their
wide sensitivity range, compact size, linear response to radiation, relative energy independence, and their
reusability. However, because a readout system is required to obtain doses from these dosimeters, they
cannot provide immediate dose information. Further, once read, the accumulated dose is effectively erased
and, consequently, there is no permanent record.

19.1.1 Thermoluminescent Dosimeters


Thermoluminescence (TL), as the name implies, is the release of photons from a substance when heat
is applied. The time when thermoluminescence was discovered is unknown, although the phenomenon
was recorded in alchemist texts dating back at least to 1602 [Arnold 1991]. The first scientific report on
thermoluminescence was presented by Robert Boyle in 1663 to the Royal Society of London [Becker 1973],
where he described glimmering light from diamond samples when heated. TL was first used as early as 1895
by Weidemann and Schmidt to detect ionizing radiation. Hence, the thermoluminescent phenomenon has
been known for quite a while.
The physical aspects of thermoluminescence were studied by many researchers after the pioneering work
of Weidemann and Schmidt, and include, for example, work by Randall and Wilkins [1945], Boyd [1949],
and numerous references provided in Becker [1973] and Horowitz [1984a]. However, it was not until 1954
that Farrington Daniels, after studying the radiation effects of thermoluminescent minerals [Daniels et al.
1949; 1953; Daniels and Saunders 1950; see also Boyd 1949; Saunders et al. 1953], suggested the use of
thermoluminescent materials, particularly LiF, as dosimeters [Morehead and Daniels 1957; Cameron 1991].
Several additional thermoluminescent materials have since been studied as dosimeters as well, including
CaF2 , CaSO4 , and Li2 B4 O7 [Kossel et al. 1954; Ginther and Kirk 1957; Hecklesberg and Daniels 1957;
Schulman et al. 1967].

949
950 Luminescent, Film, and Cryogenic Detectors Chap. 19

General Operation
diffusion electron Thermoluminecesnce involves two main processes:
(1) radiation absorption with subsequent electron
EC
trapping, and (2) electron and hole recombination
shallow
electron with light emission. During the absorption pro-
trap hn cess, TL materials absorb energy from ionizing ra-
prompt
deep
wide electron emission diation and excite electron-hole pairs. These elec-
fading
band trap
gap trons and holes diffuse through the crystal, much
hole
traps as they do in a scintillator, and during their mi-
gration they can recombine or fall into electronic
ion
E V traps located in the band gap (see Fig. 19.1). How-
diffusion hole izin
gr
ad ever, unlike scintillators that rapidly release pho-
iat
ion
tons via fluorescence, thermoluminescent materials
Figure 19.1. Band diagram depicting electronic trapping and undergo a delayed release of photons and should
emission during the irradiation and storage time. more correctly be referred to as phosphorescence.
shallow traps are The phosphorescence emission time is a function
1 2 3 2 4 1 cleared in pre-heat of the trap energy. Shallow traps tend to release
EC
charge carriers in a relatively short period of time
while deep traps can retain charge carriers for long
hn periods of time, in some cases for many decades.
very deep traps are
cleared in anneal These storage traps can be designed into the mate-
rial by adding select amounts of specific impurities.
If the trap is unstable, or shallow, recombina-
EV tion may occur at room temperature, an effect often
Figure 19.2. Band diagram depicting detrapping and emis- termed as “fading”. However, the stable deeper traps
sion during the heating time. The shallow traps (1) are emptied retain charge carriers provided that they do not ab-
during the preheat phase. After preheat, the PMT counter is sorb enough energy to excite the electrons or holes
activated and the total photon yield is integrated as the traps
release charges in order of trap energy (2, 3, and 4). These back into the conduction or valence bands, respec-
deeper traps are used to provide a reading of the accumulated tively. When energy is deposited in a TL material,
dose. After the read time, the counter is deactivated and the trapped electrons and holes may acquire sufficient en-
TLD temperature is increased to release charges from the deep- ergy to be dislodged and allow them to return to the
est traps.
conduction or valence bands, respectively, and then
rapidly recombine at a luminescent center. As these electrons and holes recombine, the excess energy is
released as UV or visible light as shown in Fig. 19.2. By recording the number of photons released with a
light sensor (such as a photomultiplier tube), the number of trapped charges can be measured. Ultimately,
the total number of photons detected gives a measure of the sample radiation dose.
The governing differential equations that predict the dynamic behavior of a TLD are generally coupled
and non-linear. Only for simple models, and even then with restrictive assumptions, are analytic solutions
possible. Nevertheless, much can be learned from these simple models. Below a few simple TLD dynamic
models are summarized.

Modeling the Thermoluminescence Intensity


Randall and Wilkins [1945] proposed a model for luminescent output from a thermoluminescent dosimeter
(TLD).1 In their model all of the electron traps are at a single energy Et below the conduction band. The

1 See also Garlick and Wilkins [1945].


Sec. 19.1. Luminescent Dosimeters 951

probability per unit time of releasing an electron from a trap back to the conduction band is

−Et
p = ω exp , EV < Et < EC , (19.1)
kT
where ω is a frequency factor associated with the trap, and k and T have their usual meanings. Randall and
Wilkins [1945] explain that the trapped electron is like a particle in a potential box and that the frequency
factor ω is the product of the frequency with which the electron strikes the sides of the box times the Mott
and Gurney [1948] reflection coefficient. Alternatively, ω can be thought of as the frequency with which a
trapped electron interacts with the lattice phonons times a transition probability. The frequency factor ω
can never be greater than the lattice vibrational frequency and is usually several orders of magnitude less
than this limiting frequency, i.e., ω  1013 s−1 [Mott and Gurney 1948; Randall and Wilkins 1945].
If Nte (t) is the density of electrons located in traps
pre-heat read at time t, then the average number of trap releases per
luminescence

temperature unit time per unit volume is Nte (t)p or

dNte (t) −Et


anneal − = Nte (t)ω exp . (19.2)
dt kT

If the emitted electrons are not retrapped, then the in-


tensity of the thermoluminescent glow is proportional to
temperature the electron release rate, i.e.,
Figure 19.3. Depiction of a temperature-dependent glow dNte (t) −Et
curve from a TLD with multiple trap energies, showing the I(t) = −C = CNte (t)ω exp , (19.3)
three regions of operation for the TLD reader.
dt kT

where C is a constant describing the luminescent efficiency and volume of the TLD. If the TLD is heated at
a uniform rate
dT
RT = , (19.4)
dt
the independent variable t can be replaced by T through dt = (1/RT ) dT so that Eq. (19.3) can be written
as
dNte (T ) ω −Et
=− exp dT. (19.5)
Nte (T ) RT kT
If Nte (T0 ) is the density of electrons in traps at time t0 and temperature T0 , then Eq. (19.5) can be
integrated to find
 T
Nte (T ) ω −Et
ln =− exp dT  . (19.6)
Nte (T0 ) RT T0 kT 
Substitution of the result of Eq. (19.6) into Eq. (19.3) yields

dNte (t) dNte (T ) dT dNte (T )


I(T ) = −C = −C = −C RT
dt dT dt dT
  T 
−Et ω −Et
= Nte (T0 )C ω exp exp − exp dT  . (19.7)
kT RT T0 kT 

Equation (19.7) describes the emission of a temperature-dependent glow curve of a TLD. Figure 19.3 shows a
typical glow curve for a TLD with multiple trap energies and Fig. 19.4 shows results for the above model of a
952 Luminescent, Film, and Cryogenic Detectors Chap. 19



   

 




!
"


     
 
Figure 19.4. Theoretical glow curves versus temperature for phosphors with a single
trap level, assuming no retrapping of electrons, after irradiation at T = 90 K with
RT = 2.5 ◦ C/sec. Parameters for the various cases are:
(A) Et = 0.3 eV, ω = 109 s−1 ; (B) Et = 0.4 eV, ω = 109 s−1
(C) Et = 0.4 eV, ω = 108 s−1 ; (D) Et = 0.4 eV, ω = 107 s−1
(E) Et = 0.6 eV, ω = 109 s−1 ; (F) Et = 0.8 eV, ω = 109 s−1
(G) Et = 0.4 eV, ω = 106 s−1
After Garlick and Gibson [1948].

TLD with a single trap energy. The maximum intensity Imax for a glow peak can be found by differentiation
of Eq. (19.7) with respect to T and setting the result to zero. In this manner, the temperature Tm at peak
luminosity is found from the relationship
Et ω −Et
2
= exp . (19.8)
kTm RT kTm

There are several properties that can be gleaned from Eq. (19.7) and Eq. (19.8) [Garlick 1949]. First,
the temperature of the glow peak maximum increases with Et for constant values of ω and RT . Second, as
the heating rate RT is increased or the value of ω is decreased, the glow peak shifts to higher temperatures
for constant values of Et . For any constant value of filled trap states Nte (T0 ), the total luminosity, the area
of the glow curve, should remain constant, although the shape changes with ω, Ete , and RT . Finally, at low
temperatures (T  Tm ), the initial portion of the glow curve should follow the prediction of Eq. (19.3).
Schayes and Brooke [1963] derived an expression for the maximum luminosity that includes the effects
of total dose and heating rate,
 ∗ ∗ 2

k e−1+2u −6(u )
Im  RT Nte (t0 ) , (19.9)
Et (u∗ )2

where the dimensionless temperature at the glow curve maximum is u∗ = (kTm )/Et . From Eq. (19.9), it
would seem that the maximum output intensity would remain constant provided that the radiation exposure
Sec. 19.1. Luminescent Dosimeters 953

is adjusted to be proportional to 1/RT . In other words,


if Nte is linearly adjusted to exactly counter the effect of
RT , the glow peak maximum output is constant. These
predictions were tested with experiments performed by
Gorbics et al. [1969], in which glow curves were mea-
sured for CaF2 :Mn, natural fluorite, LiF (TLD-100),
CaSO4 :Mn, Li2 B4 O7 :Mn, and lithium aluminosilicate
(LAS) glass. The glow curves were obtained at different
heating rates for different gamma-ray exposures. The
important results indicate that thermal quenching oc-
curs for rapid heating rates, consequently reducing the
total light yield and maximum light intensity. Shown in
Fig. 19.5 and Fig. 19.6 are temperature and time depen-
dent glow curves, respectively, for CaF2 :Mn (TLD-400) Figure 19.5. Glow curves versus temperature for
at several different heating rates. The TLDs were ex- CaF2 :Mn for eight different heating rates. For each case
posed to gamma rays from 60 Co for a time proportional the gamma-ray exposure was adjusted to be proportional
to 1/RT , an adjustment which should lead to a nearly con-
to 1/RT . The results should yield identical peak max- stant glow curve maximum given by Eq. (19.8). Data are
ima but, as can be seen from the results of Fig. 19.5 and from Gorbics et al. [1969].
Fig. 19.6, do not. The deviation from Eq. (19.9) is a
consequence of TLD thermal quenching [Gorbics et al.
1969].
Attix [1986] points out a few other properties that
can be seen from the results of Fig. 19.5 and Fig. 19.6.
First, the length of time required to reach the glow peak
maximum is nearly inversely proportional to the heating
rate. Second, for heating rates below 40◦ C per min,
the glow curve areas, as a function of temperature, are
nearly identical. Yet, the dose for these glow curves
was decreased by a factor of 10 as the heating rate was
increased from 4◦ C per min to 40◦ C per min. At heating
rates greater than 40◦ C per min, the glow curve area is
observed to decrease. Third, the glow curve area as a
function of time is observed to be nearly proportional Figure 19.6. Glow curves versus time for CaF2 :Mn for
to the dose for heating rates less than 40◦ C per min. eight different heating rates. For each case the gamma-ray
Fourth, the glow curve peak temperature increases with exposure was proportional to 1/RT . Data are from Gorbics
et al. [1969].
heating rate. Finally, for CaF2 :Mn, the temperature for
the onset of thermal quenching was approximately 290◦C. Overall, for dosimetry purposes, it was concluded
by Attix that the total light emission over time is a superior dose metric, compared to the light emission
maximum, because there is a smaller error associated with fluctuations in the heating rate.
For most TLDs there are numerous levels of electron and hole traps that are mostly designed into the
TLD by purposely adding dopants that act as traps and luminescent centers. The photons emitted from the
multiple traps can be added to produce the total luminescent glow. Hence, the glow curve is described by
[Leverenz 1950],

  T 

M
Eti ωi Ei 
I(T ) = i i i
Nte ωC exp − exp − exp − t  dT , (19.10)
i=1
kT RT T0 kT
954 Luminescent, Film, and Cryogenic Detectors Chap. 19

where the superscript i identifies the trap and properties and M is the number of different trap levels. Lumi-
nescent centers that are close in energy may not be resolved and, thus, cause the appearance of asymmetric
and wider glow peaks.
For the derivation of Eq. (19.7), Randall and Wilkins [1945] assumed that no electron retrapping occurred
once excited from traps. Garlick [1949] considered a simplistic case for retrapping, for which detrapped
electrons have equal probability of falling into either luminescent centers or empty trapping centers. For
simplicity, assume that the material has one type of trapping center distributed uniformly with density Nt .
Further, it is assumed that there are no empty luminescent centers2 in the unexcited phosphor. The density
of filled trapping centers is Nte and the density of empty trapping centers is Nt0 ; hence
Nt0 = Nt − Nte . (19.11)
If the material is an insulator, and most TLD materials are, the density of electrons in the conduction band
should be considerably less than the density of trapped electrons Nte . Heating causes centers to depopulate
so they become a source of electrons for the traps. Hence, the density of trapped electrons becomes the same
as the density of empty luminescent centers (Nte = N0 ).3
For a density of electron-filled traps of Nte , the probability that a detrapped electron falls into a lumi-
nescent center, which has a density of Nt , is
Nte Nte Nte
p= = = . (19.12)
Nt0 + N0 (Nt − Nte ) + Nte Nt
Equation (19.12) indicates that when few traps are populated, then there is a low probability that detrapped
electrons recombine at luminescent centers. Further, if the traps are completely populated, i.e., Nte = Nt ,
a detrapped electron has no option but to recombine at a luminescent center. From this interpretation,
Eq. (19.2) is modified to
dNte (t) Nte (t)2 −Et
− = ω exp . (19.13)
dt Nt kT (t)
Note that it is assumed in Eq. (19.12) and Eq. (19.13) that the capture probabilities of the trap and luminous
centers are equal, but this is an assumption that may not be true.
To solve the above separable differential equation, first change the independent variable to T with the
use of Eq. (19.4). The solution is
$  T /−1
1 1 ω Et 
Nte (T ) = + exp −  dT . (19.14)
Nte (T0 ) Nt T0 RT kT
From this result the thermoluminescent intensity I as a function of temperature, which is increased at a
uniform rate [Garlick and Gibson 1948], is
Nte (T0 )2 −Et
C
ω exp
dNte dNte dT Nt kT
I(T ) = −C = −C =  T 2 . (19.15)
dt dT dt Nte (T0 ) ω −Et
1+ exp dT 
Nt T0 RT kT 

2 An imperfection in the crystal responsible for luminescent emissions. In the present case, these imperfections are hole traps.
When occupied by an electron, they are not capable of producing light from recombination. If the electron is excited from
the center, then it is effectively occupied by a hole. An electron recombining with a hole at the luminescent center releases a
photon.
3 Garlick and Gibson [1948] appear to use the condition that the only significant source of trapped electrons is from depopulated

luminescent centers.
Sec. 19.1. Luminescent Dosimeters 955






   




 

 $
!

 " #
% &


     
 
Figure 19.7. Theoretical glow curves versus temperature for phosphors with a single
trap level, including the effects of electron retrapping, after irradiation at T = 90 K with
RT = 2.5 ◦ C/sec and ω = 109 s−1 . Parameters for the various curves are as follows:
(A) Et = 0.4 eV, Nte (0) = NT (B) Et = 0.6 eV, Nte (0) = NT
(C) Et = 0.8 eV, Nte (0) = NT (D) Et = 0.4 eV, Nte (0) = 0.5NT
(E) Et = 0.6 eV, Nte (0) = 0.5NT (F) Et = 0.8 eV, Nte (0) = 0.5NT
(G) Et = 0.4 eV, Nte (0) = 0.25NT (H) Et = 0.6 eV, Nte (0) = 0.25NT
(I) Et = 0.8 eV, Nte (0) = 0.25NT (J) Et = 0.4 eV, Nte (0) = 0.1NT
(K) Et = 0.6 eV, Nte (0) = 0.1NT (L) Et = 0.8 eV, Nte (0) = 0.1NT
After Garlick and Gibson [1948].

Example results of Eq. (19.15) are shown in Fig. 19.7 and a few characteristics are observed. First, for
constant values of Nte (T0 ), ω, and RT , the temperature of the luminescent peak maximum increases nearly
proportional with the trap energy. Second, for constant values of Nte (T0 ) and Nt , the temperature of the
luminescent peak maximum increases with RT or decreases with ω. Third, the area under each curve is
proportional to the number of initial trapped electrons, or Nte (T0 )/NT . Further, the shape of the glow curve
and position of the maximum is also a function of Nte (T0 )/NT . Finally, at low temperatures, the integral
in the denominator portion of Eq. (19.15) is much smaller than unity, and the beginning of the glow curve
should follow
ω −Et
I(T )  C [Nte (T0 )]2 exp , (19.16)
Nt kT

a prediction that differs slightly from the result of Eq. (19.3).


A much more rigorous treatment on retrapping is offered by Halperin and Braner [1960], which leads to
[Horowitz 1984a],

ωAm −Et
I(T )  C [Nte (T0 )]2 exp , (19.17)
Nt An kT
956 Luminescent, Film, and Cryogenic Detectors Chap. 19

where An is the probability of falling, into a trap while Am is the probability of recombining at a luminescent
center. Note that Eq. (19.17) is the same result as Eq. (19.16) for Am = An , as originally assumed in the
model of Garlick and Gibson [1948].
These models, as earlier stated, serve to provide a basic understanding of the thermoluminescent process.
Yet, as pointed out by Bos [2001], the actual thermoluminescent process can be complex, meaning that the
absorption and decay processes can deviate from these ideal cases. For instance, the luminescent centers may
be complex defect structures that are difficult to identify or characterize. In some cases, the defects may not
be stable when heated. Overall, to help mitigate the impact of these physical issues, Bos [2001] recommends
that the steps taken to measure the radiation dose be carefully controlled, including the irradiation process,
read-out, and annealing.

TLD Systems A TLD response is measured with a TLD reader. There are many different models, but
all have a few features in common (see Fig. 19.8). A TLD reader has a drawer unit that may have a small
containment
filament pan that a TLD chip may be placed upon, or it
may have a cradle that the inner part of a TLD badge
may be inserted. The drawer is shut in a light-tight
counter/ signal HV power enclosure with a backfill gas flowing into the chamber,
to computer output supply
(optional) usually N2 or Ar.
The backfill gas is necessary to prevent background
temperature
signal
luminescent from TLD surface contamination, such a ox-
idation, during the heating process. After the chamber is
temperature
purged of air, usually about a minute, the TLD reader is
controller activated to operate in the regions depicted in Fig. 19.3.
PMT
The TLD is heated, usually by a current flowing through
the resistive filament pan or through radiant heating of
the pan. A thermocouple is used to measure the pan
optical
filters temperature and provide feedback in order to control
planchet TLD chip the filament temperature during the heating process. A
gas
output
gas photomultiplier tube (PMT) is used to record the light
input
power
supply
output from the TLD. Optical filters are placed between
thermocouple the TLD and the PMT to reduce contamination from
signal to power spurious light emissions during the readout process. The
current from the PMT is a measure of the light emission
and, thus, is also a relative measure of the dose received
Figure 19.8. The basic components of a TLD reader.
by the TLD. This current is recorded and displayed as a
glow curve on a monitor. The TLD reader itself may have a built-in display or, more frequently, is connected
to a computer with a display monitor. The system is programmable with a variable stage input so that the
user can select the temperature range, temperature ramp rate, temperature hold times, and temperatures
between which the electronic output is measured.
Low energy traps are unreliable for dosimetry because they release electrons at room temperature, an
effect referred to as trap leakage. Consequently, the light emission from shallow traps is a strong function
of TLD storage time after the TLD irradiation. To avoid measuring the emissions from these shallow traps,
current from the PMT is not recorded until a preset threshold temperature is reached that is sufficient to
empty these traps. The TLD reader increases the temperature of the sample up to the lower threshold
temperature and then begins recording the current, or accumulated charge, from the PMT output. This
initial heating phase is called the preheat step. A typical lower threshold temperature is approximately
150◦ C, but varies with the TLD material selected. Above the low temperature threshold, the current
Sec. 19.1. Luminescent Dosimeters 957

and total charge from the PMT is recorded and, in some 

systems, the glow curve is displayed. Because the PMT &'$%() & * # $%

    


  +
!'   !' $% 
 !"# $%

is an amplification device, the total charge measured is 

an amplification of the total number of initial electrons 


producing thermoluminescence. Under constant operat-
ing conditions, it is expected that the measured charge 

is proportional to the actual TLD dose so the dose can


be determined by multiplication of the measured charge 

by a scaling constant. At a high temperature thresh-



old or limit, the TLD reader stops recording the output
but continues to heat the TLD in order to clear the deep 
traps. A typical higher threshold temperature is approx-      
  
imately 300◦ C, enough to clear the important dosime-
try traps for most TLD materials, although this limit Figure 19.9. Emission spectra from several TLD phos-
may be set higher for certain TLDs that have important phors normalized to a peak intensity of 100 per unit wave-
glow curvs features above 300◦ C. Although deeper traps length. Data from Fowler and Attix [1966] and Gorbics
[1966].
could be useful because of their long-term electron stor-
age properties, spurious infrared emissions from the heated TLD and surroundings can leak into the PMT
and produce an exaggerated dose. For reliability reasons, deep traps are usually not included in the dose
measurement. After the anneal step, the heating is terminated and the TLD is allowed to cool. It is impor-
tant that the fill gas continues to flow as the TLD is cooled to avoid oxidation and possible TLD damage.
A typical operating temperature range may go up to 400◦C to clear the deep traps. Properties of some of
the most widely used TLDs are given in Table 19.1.
From the results of Gorbics et al. [1969], it is clear that precise control of the heating rate is important for
reliable and repeatable TLD dosimetry results. An established calibration method should be used to ensure
that the measured charge corresponds to a known dose standard. Further, the temperature measurement
of the pan must be rapid and accurate so that the reader measures current during the proper temperature
limits. Although this precaution may seem insignificant, the pan temperature may differ from the actual
TLD temperature (an insulator) or that of the thermocouple. This precaution is especially important for
rapid heating rates. It was seen in Sec. 14.1.6 that the voltage has a strong influence on the gain of a PMT,
so the TLD output should be compared periodically with a calibrated TLD phosphor to ensure that gain is
constant and with insignificant variance. The TLD reader enclosure is sealed when the pan drawer is closed,
and should be kept in such manner when not in operation to avoid contamination of the optical surfaces in
the system. Further, to avoid possible reader damage, the system gas should be used to purge the enclosure
of air before operating the heater.
Emission Spectra As with scintillators, it is preferable to use TLD phosphors with emission spectra that
match well with the response functions of widely available photo-multiplier tubes. Shown in Fig. 19.9 are
the emission spectra for some common TLD phosphors. It is notable that LiF:Mg,Ti (TLD-100) matches
well to common bi-alkali PMTs. CaF2 :Mn, CaSO4 :Mn, and Li2 B4 O7 on the other hand do not match well to
common PMTs. However, their peak wavelengths near 500 nm and 600 nm present interesting possibilities
for TLD readout systems based on Si diode technology, including silicon photomultipliers (SiPMs). The
drawback is that long wavelength readout systems also have increased sensitivity to long wavelength photons
from infrared emissions, a source of background from the heating process.
Sensitivity Sensitivity is determined by the amount of light released per unit energy absorbed in the TLD.
The lower limit of detectable light emission is a function of the TLD reader and, thus, also determines the
lower limit of detectable ionizing dose. The photoelectric process dominates at low energy, especially with
958

Table 19.1. Common thermoluminescent materials used for radiation dosimetry.

Atomic Emission Useful Sensitivity Max


Density Temp. Main Energy Fading
Designation Material Number −3 Spectrum Dose to that of Temp
(g cm ) Peak (◦ C) Response* at 20◦ C
(Z) Range (nm) Range (R) TLD-100 (◦ C)

TLD-100 nat. LiF:Mg,Ti 3/9 2.635 350–600 195 10−3 – 105 1 1.35 400 5%/yr
TLD-100H, 240
nat. LiF:Mg,Cu,P 3/9 2.635 380–400 10−5 – 1.4×103 30 1.35 5%/yr
GR-200

10%/1 day
TLD-200 CaF2 :Dy 20/9 3.18 483–577 180 10−5 – 106 30 13
16%/2 wks
TLD-300 CaF2 :Tm 20/9 3.18 13
10%/16 hrs
TLD-400 CaF2 :Mn 20/9 3.18 440–600 260 10−3 – 3×105 10 13
15%/2 wks
TLD-500 Al2 O3 :C 13/8 3.987 72 3.5 400
TLD-600 95.6% 6 LiF:Mg,Ti 3/9 2.545 350–600 195 1 1.35 400
TLD-600H 95.6% 6 LiF:Mg,Cu,P 3/9 2.545 400 1.35 240
TLD-700 7 LiF:Mg,Ti 3/9 2.653 350–600 195 1 1.35 400
TLD-700H 7 LiF:Mg,Cu,P 3/9 2.653 400 12 1.35 240
TLD-800 Li2 B4 O7 :Mn 3/5/8 2.4 530–630 200 10−3 – 106 0.15 0.8
2%/1 mon
TLD-900 CaSO4 :Dy 20/16/8 ∼2.96** 480–570 220 10−6 – 105 20 12
8%/6 mon

CaSO4 :Mn 20/16/8 ∼2.96** 450–600 110 10−6 – 104 70 12 50%/day


BeO 4/8 3.01 150–325 200,240,290†

*Sensitivity at 30-keV photons relative to sensitivity at 1-MeV photons (60 Co).


**Affected by water content.
†Depends on preparation method.
Luminescent, Film, and Cryogenic Detectors
Chap. 19
Sec. 19.1. Luminescent Dosimeters 959

TLDs made of relatively high Z materials. Shown in Fig. 19.10 are calculated sensitivity responses to photon
energy for several different TLD materials. Note that TLDs manufactured from relatively high Z materials,
in particular CaF2 , CaSO4 , CaCO3 , SiO2 , and Al2 O3 , have a much higher response to photons below 100
keV.

Stability and Fading Low energy traps are unreliable for dosimetry because they release electrons at
room temperature, an effect known as trap leakage or fading with minor distinction. Trap leakage is short-
term electron loss to recombination from relatively shallow traps and usually occurs in hours to days after
irradiation. Fading refers to a longer term loss of electrons from
deep traps over an extended period of time. Both cases are 

primarily due to thermal vibration of the crystal lattice from the

ambient temperature causing the ejection and recombination of 
electrons. Consequently, the TLD reader is usually programmed  


to clear shallow traps before the system begins recording the
electronic signal from the PMT. 
 

Recall the probability of electron emission from a trap, de-  
 

scribed by Eq. (19.1), has a strong temperature dependence. The  !



half-life of the trap is defined as the time for the filled population  !"  !"
to emit half of the electrons  

 


  
ln(2) ln(2) Et
t1/2 = = exp , (19.18)
p ω kT Figure 19.10. Theoretical sensitivity of TL
phosphors as a function of photon energy, cal-
culated as a function of ratio of the energy de-
where p is the emission probability and ω is the frequency factor.
posited in the phosphor to the energy deposited
Energy levels shallower than approximately 1 eV fade rapidly, in tissue. Data combined from Cluchet and Joffre
while energy levels exceeding 1.5 eV are generally long lived, [1965] and Scarpa [1970].
even with large frequency factors [Shani 1991].
Methods to reduce the effect of fading include a pre-irradiation anneal to clear the traps and reduce their
relative contribution to the glow curve. After irradiation, a pre-heat step is routinely performed to empty
these traps before the PMT is used to record the thermoluminescence. For most TLDs, the pre-heat step
is performed for temperatures below 150◦ C, although this temperature threshold may vary with the TLD
material. Storage of the TLDs in darkness at cool temperature can reduce fading. However, because shallow
traps are still unreliable as a dosimetry record, mainly due to fading during the exposure period, the pre-heat
step is still recommended.

Superlinearity and Sensitization At low radiation doses, the response of TLD phosphors is nearly linear.
However, at high doses the response of a TLD deviates from linearity and becomes supralinear as shown
in Fig. 19.11. The threshold for supralinear behavior is a function of the phosphor types, occurring at
approximately 10 röntgens (R) for Li2 B4 O7 :Mn and as high as 104 R for CaF2 :Mn. At excessive doses the
thermoluminescence decreases with dose.
If one simply regards the retrapping model of Garlick and Gibson [1948], the luminescence would be
expected to increase as Nte (T0 ) → Nt , because the electrons are more likely to fall into luminescent centers
than traps that are already filled with electrons, a prediction that can be observed from Fig. 19.7. Hence, the
luminescent efficiency should increase with dose. At some degree of irradiation, the traps become saturated
and no additional electrons can be stored in the traps. Consequently, the TLD material reaches a luminosity
limit. Additional irradiation can cause damage to the material, thereby introducing more defect centers
that act as traps that compete with the luminescent centers and consequently reduce the luminosity. The
supralinear effect for several TLD materials is shown in Fig. 19.12.
960 Luminescent, Film, and Cryogenic Detectors Chap. 19



&'()*+


&,*+-.

     !"  #


' (
saturation 


$ %  


,*+
sublinear 
/(*0 /(*+
 1(*
Thermouminescence

region


supralinear
region





linear

region 
    
      
   

Figure 19.12. Thermoluminescent growth


curves for several common TLD materials. The
D1 D2 Dose graphs were all normalized at 100 R. Data are
from Attix [1986]; Lakshmanan et al. [1981]; Mar-
Figure 19.11. Representation of thermolumi- rone and Attix [1964]; Portal et al. [1980]; Sunta
nescent growth curve depicting the linear, supra- et al. [1971]; Tochilin et al. [1969]; and Wilson
linear, sublinear, and saturation regions. and Cameron [1968].

 Sensitization is the process whereby a TLD becomes more


 sensitive to radiation (S/So ) after exposure to a large radi-
ation fluence. Here S is the sensitivity after the process

and So is the response for unsensitized samples. The pro-
 


 
duction of additional traps from radiation damage makes a
 TLD produce more light as a function of radiation expo-

! sure, as shown for Li2 B4 O7 :Mn in Fig. 19.13. S/So values

of 5 can be achieved with TLD-100 [Horowitz 1984b]. The

sensitization process is different for each type of TLD mate-

rial. For instance, Cameron et al. [1968] describe a process
 in which LiF is irradiated to about 105 R and subsequently
      
  annealed at 300◦ C for an hour. Sensitization can lead to
increased linearity over a wider range than that observed
Figure 19.13. TL as a function of exposure for with an unsensitized sample, and TLDs may be purposely
Li2 B4 O7 :Mn before and after radiation-induced sensi-
tization from exposure to 60 Co gamma rays. Data are sensitized to take advantage of this property. However, the
from West [1967]. deep traps produced during the process may become a source
of low background phosphorescence, a nuisance for low-level
dosimetry measurements [Horowitz 1984b]. Mayhugh and Fullerton [1975] describe a method to reduce inter-
ference effects of deep levels on low exposure measurements, in which TLD-100 samples are illuminated with
UV radiation while being annealed at 300◦ C. Such samples retain high sensitivity while remaining useful in
the mR range.

Radiation Damage The response of TLDs declines at higher radiation exposures than used for sensitization,
usually greater than 105 R [Cameron et al. 1968; Shani 1991]. Multiple models have been proposed for the
high radiation behavior observed for TLDs that involve the formation of competing trap centers in the
materials [Horowitz 1984b]. If a significant density of shallow traps are created from radiation damage,
Sec. 19.1. Luminescent Dosimeters 961

they effectively accumulate electrons that might otherwise lodge in the useful phosphorescent centers. These
shallow traps are neglected during the measurement process, and consequently the overall signal decreases
below the predicted linear output. If deep traps are introduced by radiation damage, they also do not
contribute to the glow curve signal because they require higher temperatures to depopulate. In either case,
the competing traps emit electrons at temperatures outside of the read region depicted in Fig. 19.3. This
radiation damage may be permanent and cannot be removed by annealing. Further, at high doses, electrons
filling the usual phosphorescent centers can cause a saturation effect, in which the probability of filling these
useful centers diminishes as fewer become available. At high radiation doses, TLDs become discolored, an
indicator of significant radiation damage. With increasing radiation exposure, TLDs change in appearance
from translucent white, to yellow, brown, dark brown, and eventually to black. The formation of these color
centers causes re-absorption of luminescent photons, resulting in a decrease in light output. Overall, the
useful linear range of most TLDs is from tens of mR up to approximately 103 R, and the useful sensitized
range is from hundreds of mR up to approximately 105 R. The thermoluminescent intensity as a function of
dose for several TLD materials are compared in Fig. 19.12.
Calibration Calibration procedures are based on comparisons between known TLD radiation exposures and
the response of unknown TLD exposures. The procedure requires a number of stringent controls, including
sample size and mass, calibration standard location with respect to the radiation source, and temperature
and time control of the glow curves. Further, it is important that the actual TLD reader be maintained by
periodically verifying the correct response to a known TLD exposure (dose).
Calibration generally consists of irradiating a TLD with a known dose and calibrating the TLD reader
to correlate the glow curve output with that known dose. Suppose that the sample dosimeter is deployed
and irradiated in a known environment with a known dose of Dk and produces a glow curve response of Rk .
Then a simple calibration factor becomes
Dk
fD = . (19.19)
Rk
Given an unknown exposure of ionizing radiation to a dosimeter under the same conditions, the unknown
dose Du is a function of the glow curve response Ru , and is determined from

Du = fD Ru . (19.20)

If the same TLD chip is used for the calibration and then, shortly after being cleared, is used for dosimetry
measurements, then the correlation seems straightforward. However, complexities arise from the non-linear
response of TLDs to gamma-ray energies as shown in Fig. 19.10. The identified dose may be incorrect
unless the same radiation type and energy are used for both the calibration and the measurement. Further,
because TLDs are often used to determine dose, a correction must be made to relate the TLD response to
that which would occur within tissue (or bone). The outcome becomes even more complicated because the
response of a TLD changes with accumulated dose, storage time, thermal history, and even the environment.
Consequently the value of fD must be measured periodically.
If the individual TLDs are also calibrated, this process may account for variances in the TLD output.
However, complications can arise if a general average response for a type of TLD is used for calibration to
characterize additional TLDs of supposedly the same type. Clearly such an assumption can promote error,
mainly because of variances in the responses between individual TLD chips.
To correct the response for different radiations and energies, the TLD can be exposed to various sources
and the independent values of fD can be recorded. However, this cumbersome method is usually replaced
by calibrating the TLD with a single reference source. For instance, the source in the calibration table of
Fig. 19.14 is 137 Cs, while another common source is 60 Co. This reference source can be used to determine a
reference dose Dr and the resulting reference TLD reader response Rr . This result can be directly compared
962 Luminescent, Film, and Cryogenic Detectors Chap. 19

Figure 19.14. A dosimetry calibration table in a low scatter environment. (left) A 137 Cs source is
stored in the shield below the table. (right) The source is raised through the port stem when in use.
Concentric rings increasing by 10 cm radial increments mark placement locations.

to the known dose at the working location, where the badge is deployed, to find a relative scaling factor ηr .
The calibration factor for the reference source is

fr = Dr /Rr . (19.21)

The relative response is defined as


ηr = fD /fr , (19.22)
which gives the user a method to calibrate TLDs from the reference source. For high energy electrons
and gamma rays, above 300 keV, the response is almost constant for most TLD materials, hence ηr is also
essentially constant. For lower energies, this simply is not true. Further, at high doses, the TLD may become
sensitized, thereby also changing the response. Consequently, the reference source can be used only for a
limited energy range and dose.
A calibration system typically consists of a table, preferably made from low Z material such as plastic
or wood to minimize photon scattering, that contains a port for a gamma-ray source. The gamma-ray
source is stored in a radiation shield below the table, and is mechanically raised up through the port to
expose the calibration TLDs placed at various distances from the port. Although 60 Co is a source frequently
used for calibration, 137 Cs and 226 Ra are also widely used. Source strengths of a few mCi are often used
to reduce statistical uncertainty and exposure time. The table is usually circular with concentric distance
markings surrounding the source port. These tables typically are between 2 to 4 meters in diameter. If the
source-to-TLD distance is greater than 2 m, air scattered photons may become significant and can skew the
calibration from the ideal, point-source, uncollided flux model usually assumed in the calibration process.
Likewise placement of the TLDs too close to the source may introduce complexities arising from the finite
source size and uncertainties in the solid angle of irradiation. Hence, TLDs are usually placed a distance of
10 cm to 2 m away from the source port. In Fig. 19.14 an example of a TLD calibration table is shown.
The calibration system is placed in an empty room of such size that the detectors are always much closer
to the source than the floor, ceiling or walls. This precaution minimizes the TLD absorption of scattered
gamma rays. The TLDs should be placed at known locations from the source, horizontally and vertically,
usually on premarked lines on the table as shown in Fig. 19.14(right). The gamma-ray exposure for each
TLD can then be calculated from the known source activity based on an uncollided photon flux model to
produce a calibration curve.
The TLD reader can also suffer from slight changes in light sensitivity, also causing error in the dose
measurement. Lindskoug and Lundberg [1984] recommend testing the TLD reader as often as each day
(presumably for daily usage of the instrument) with a constant light source. They also suggest the use of
Sec. 19.1. Luminescent Dosimeters 963

a TLD dosimeter as that light source, irradiated at a constant known dose beforehand, used each day and
stored in a refrigerator between uses. This new calibration factor fL is multiplied by Eq. (19.20) to correct
for TLD reader response changes. Overall, the measured dose can be determined with

Du = ηr fL fr Ru . (19.23)

Some TLDs, such as LiF, have a density close to that of tissue, which explains, in part, the popularity
of LiF. In other words, the light yield from the glow curve must be calibrated to the dose in tissue. A
simple correction method is to assume that the dose of the TLD is related to tissue dose by ratio of the
mass collisional stopping powers. Energy deposition is also a function of radiation type. Shani [1991]
presents several formulations describing the relation between dose and TLD response for different radiations,
including electrons, heavy charged particles, gamma rays, and neutrons. Many are sensitive to both neutrons
and gamma rays, while others have almost no sensitivity to neutrons; hence, by strategically pairing different
TLDs, separate gamma-ray and neutron doses can be determined.
TLD Forms
Thermoluminescent materials are available in many physical forms such as powder, compressed ribbon,
dispersed in Teflon, pellets, plates, and single crystals. Many TLD materials are initially grown as an ingot
with the activator dopant included. Unfortunately, the impurity concentration is distributed through the
crystal according to its migration coefficient and, consequently, the activator concentration varies throughout
the crystal. If TLDs are sliced directly from such an ingot, they usually have a wide variation in radiation
response. To avoid this variability, the ingot is often ground into powder, usually with an average grain size
of about 200 microns, and the powder is then thoroughly mixed to produce a uniform activator concentration
[Mayhugh 2000]. This thermoluminescent powder can be deployed in a gelatin capsule, a glass capillary, or
plastic tubing. For plastic tubing or gelatin capsules, the irradiated TLD powder is poured into a planchet
pan and read. Powder encapsulated in potassium-free glass capillaries can be read in the capsule. The more
convenient and commercial TLD forms have the powder hot-pressed into solid ribbons, rods, or sliced into
small chips and disks. These forms are easy to handle and can be placed directly on the heater planchet for
readout.
Often the sensitivity or stability of some TLD materials is improved when embedded in an inert material
such as Teflon. The TLD powder is mixed with the inert material and then compressed into pellets or chips
with thicknesses of about 100 to 300 microns. These chips can be inserted into containers that are inserted
directly into the TLD reader. Finally, under special conditions, single crystal TLDs cut directly from a single
crystal ingot are sometimes used. However, because of the wide variance in doping distribution in the bulk
crystal, and variance in response among different chips, this form is unpopular for generally dosimetry.
Summary of Advantages and Disadvantages
The advantages of thermoluminescent dosimeters as a dose detector are many. TLDs are relatively inexpen-
sive and can be acquired in many different forms. By properly using established annealing methods, they can
be reused multiple times. Further, with periodic calibration, the variance in dose measurement can be kept
small. Most TLDs are made from relatively low Z materials and have a low mass density; hence, they can
be modeled as nearly tissue equivalent dosimeters. Their small size is convenient for dosimetry because they
can be modeled as point detectors. The dose measurement range is large with some TLDs being capable of
measuring radiation doses below a millirem while also being able to measure doses above 104 rem. Finally,
modern TLD readers can be connected to personal computers to provide straightforward readout and data
interpretation.
However, TLDs also have some disadvantages. First, once a TLD is read, the dosimetry information is
erased from the dosimeter and, thus, is quite different from photographic dosimetry methods. All TLDs
964 Luminescent, Film, and Cryogenic Detectors Chap. 19

fade with time, some more rapidly than others. Consequently, the luminescence is a function of storage time
and storage environment. Further, the luminescence for many TLDs is a function of the irradiation rate
as well as the total dose, and some TLDs show strong supralinearity. The output luminescence and glow
peak maxima for many TLDs are functions of the heating rate. TLDs are sensitive to UV light and proper
storage and annealing before deployment is necessary. The emission spectrum for some TLDs is mismatched
to the response function of many photomultiplier tubes and thus decreases the measured luminosity. TLDs
can have different sensitivities, even when made from similar materials. Thus each individual TLD must
be calibrated. Finally, TLD sensitivity can change after receiving large radiation doses, an effect termed as
sensitization.

Common Materials for Thermoluminescent Dosimetry


Numerous materials have been investigated as thermoluminescent materials, including many common min-
erals. In fact, there are so many that it is impractical to discuss all of them here, and authors of books
devoted to this topic seldom wander down that path. Instead, discussed here are a few common materials
successfully used as TLDs, many of which are commercially available and widely used.

Lithium Fluoride
Lithium fluoride (LiF) is the most studied of the TLD materials and also is the most popular TLD in use
today. The relatively low density of LiF is closer to tissue than most other TLD materials, an important
property for dosimeters. LiF is stable at low temperatures and is mostly chemically inert. Manufacturers of
LiF optics warn that the material is attacked by atmospheric moisture at temperatures above 400◦C.4
LiF TLDs are available with many different 7 Li enrichments and activators, the most popular being the
TLD-100, formed from natural LiF doped with Mg and Ti. Enriched and highly sensitive LiF TLDs are also
available for special applications. Those most used are listed in Table 19.1.

Although LiF can be grown as a single crystal, this
form is generally not used for TLDs. Instead, dopants
 are added to the purified LiF starting material and single
crystals are grown from a melt process, typically with
  Czochralski or Stockbarger methods. The unfavorable
    

segregation coefficient of Mg causes it to migrate dur-



ing growth (as with other activators during zone melt
purification) and, consequently, a non-uniform doping

 distribution is produced. As mentioned above, this non-

uniform activator distribution can be ameliorated by
   


  
pulverizing the crystal, mixing the resulting powder, and


 hot pressing or sintering the mixed powder into rods
      
 
and ribbons. The end product is a translucent material
with a relatively uniform distribution of the activator
Figure 19.15. The normalized glow curve and its vari- dopants. A normalized composite representation of a
ous composite components for LiF TLD-100 exposed to LiF:Mg,Ti glow curve with the separate trap luminosity
1 Gy gamma irradiation. The luminosity is in arbitrary
or relative units (a.u.). Composite data acquired and ad- components is shown in Fig. 19.15. The emissions de-
justed from Livingstone et al. [2009] and Horowitz and noted 2 and 3 in this figure are usually excluded from a
Moscovitch [2013]. measurement, typically set to begin when the tempera-
ture ramp reaches 150◦C and extends up to approximately 225◦ C. Hence, the main luminescent contributions

4 Apparently, LiF in the presence of water moisture at elevated temperatures hydrolizes and forms HF, which consequently
attacks glass.
Sec. 19.1. Luminescent Dosimeters 965

come from peaks 4, 5, 5a, and 5b. The sensitivity is linear in the range between 1 mR and 1 kR, and is
supralinear between 1 and 50 kR.
To clear the deeper traps, some care is required for proper annealing of TLD-100 dosimeters to maintain
reliable reuse. The annealing is usually performed at 400◦ C for 1 hour, followed by a slow cooling step and
a longer term (∼ 24 hours) anneal at 80◦ C. However, to prevent damage to LiF material embedded in a
temperature sensitive binder, these TLDs can also be annealed at lower temperatures ranging between 280◦
to 300◦ C [Becker 1973].
The higher temperature annealing is important to empty traps 6 through 11, thereby reducing back-
ground phosphorescence. The IR contamination of the spectrum from the heater is the reason these higher
temperature traps are not used in the dose measurement. Although fading is relatively slow, different low
fade rates arising from different annealing procedures have been reported. When the annealing method is
rigorously controlled, the fading can be limited to approximately 5 to 10% per year [McKeever 1985].
TLD-100 dosimeters are sensitive to charged particles, gamma rays, and neutrons. Gamma rays excite
primary electrons in the material through the photoelectric effect, Compton scattering, or pair production.
These energetic electrons excite secondary electrons in the material through Coulombic scattering. It is
unlikely that energetic electrons deposit all of their energy in a small TLD chip before reaching the detector
boundaries; hence, usually only a fraction of the incident energy is measured. The same is true for energetic
beta particles. However, dosimetry is based on the amount of ionization produced in the body, primarily
body tissue, and cavity theory attempts to correct for these energy losses.5
Heavy charged particles produce electron-hole pairs di-
 $
rectly through Coulombic scattering. Because natural Li 
6
has a natural abundance of approximately 7.6% Li, neu-
  






trons are also detected through the 6 Li(n,t)4 He reaction, in

  !"
which the triton and helium reaction products directly ionize 

the material. The ranges of alpha particles and heavy ions

are relatively short in LiF, usually only tens of microns, and 
most of the energy of the reaction products can be absorbed 
 
in the dosimeter. The glow curve from electrons and heavy  !"
#

ions is significantly different because a glow curve peak ap-
pears at 275◦ C from alpha particles [McKeever 1985]. Hence,  
   
the glow curve peak 7 (Fig. 19.15) is enhanced by high lin-    
ear energy transfer (LET) radiation [Budd et al. 1979]. In Figure 19.16. Comparative results for LiF TLD-
some cases, the enhanced response of peak 7 has been used 100 dosimeters, showing deviation in peak height and
to extend the sensitivity of TLD-100 dosimeters out to 107 area as a function of heating rate. The gamma-ray
exposure was adjusted to be proportional to 1/RT for
R [Jones and Martin 1968]. the peak height, while the exposure was normalized
The glow peak properties of LiF:Mn,Ti changes with for the peak area data. Also shown is the change in
heating rate, and thus, this TLD requires a calibrated and peak temperature with heating rate. Data are from
constant measurement procedure. Both the glow curve peak Gorbics et al. [1969].
height (peak 5) and the glow curve area have an output maxima near a heating rate of 80◦ C per minute
(see Fig. 19.16). Further, the thermal location of the glow peak increases with heating rate, changing from
185◦ C at a rate of 4◦ C per minute up to 225◦ C at a rate of 700◦C per minute. If operated at the luminosity
maximum, the glow peak appears near 205◦ C.
The neutron response of LiF can be enhanced by replacing the natural Li with approximately 95.6%
enriched 6 Li, and TLDs of this type are labeled TLD-600. The emission of heavy charged particles with high

5 Partof cavity theory is the assumption that an electron leaving the dosimeter is replaced by an electron leaving the surrounding
environment and into the dosimeter. This condition is known as charged particle equilibrium.
966 Luminescent, Film, and Cryogenic Detectors Chap. 19

 LET produces a glow curve with a significant increase


 in peak 7 with respect to peak 5 for neutron reactions.

With proper calibration, the ratio of peak 7 to peak 5 can
   


give a measure of the neutron dose [McKeever 1985]. LiF
depleted of 6 Li, having 99.99% 7 Li, are relatively insen-
 sitive to neutrons and are labeled TLD-700. Often TLD-
600 dosimeters are paired with TLD-700 dosimeters in a
 single dosimeter badge. By comparing the signals from
TLD-600 and TLD-700 pairs, a separate measure of the

 neutron and gamma-ray dose can be determined.
 

 The sensitivity of LiF is enhanced by changing the
      activation phosphors from a combination of Mg and Ti
  to a combination of Mg, Cu, and P, and natural LiF with
this activator combination are labeled TLD-100H (also,
Figure 19.17. The normalized glow curve with its various
components for LiF TLD-100H exposed to 5 Gy gamma
GR-200). The glow curve is different than observed with

irradiation. Data were acquired and adjusted from those TLD-100 with the main peak appearing near 200 C [Tri-
of Triolo et al. [2006]. olo et al. 2006], as shown in Fig. 19.17. Overall, these
dosimeters can usefully measure lower doses than TLD-100, ranging from 10−5 R to about 103 R. However,
they do not have the extended upper range observed with TLD-100. Further, the maximum thermal range
is limited to no more than 240◦ C or the TLD is permanently damaged. Unfortunately, this restriction also
means that TLD-100H dosimeters cannot be annealed to clear the deep traps. Eventually, after many expo-
sures, the background emissions from these deep traps can begin to interfere with low dose measurements.
A relatively new LiF TLD with Mg, Cu, Si activators is under investigation [Kim at al. 2010; Horowitz
and Moscovich 2013]. The main peak appears near 250◦C, higher than TLD-100, but still low enough to
minimize IR contamination. These LiF TLDs have similar sensitivity as the TLD-100H, but the deep traps
can be annealed without damaging the dosimeter. Kim at al. [2010] report that after a multi-step anneal
process, the residual deep trap signal is reduced to only 0.05%.

Calcium Fluoride
Calcium fluoride (CaF2 ), or fluorite, is a mineral with attractive properties for thermoluminescent dosimetry.
There are four prevalent CaF2 TLD types, namely natural fluorite, Dy-doped (TLD-200), Tm-doped (TLD-
300), and Mn-doped (TLD-400). A characteristic shared by all CaF2 TLDs is the elevated gamma-ray energy
absorption at energies below 100 keV (see Fig. 19.10), a consequence of the generally higher mass density of
CaF2 . To reduce the effect, filters can be employed to flatten the gamma-response at these lower energies.
Reviews of important CaF2 TLD properties can be found in the literature [Becker 1973; Harvey et al. 2010;
Bidyasar 2014].

CaF2 :MBLE Natural CaF2 , sometimes called MBLE CaF2 , was studied extensively and was a commercial
TLD product for many years.6 However, CaF2 :natural is far from an ideal TLD material because material
obtained from different sources can have significantly different glow curves as shown in Fig. 19.18. Peaks in
the glow curves, labeled in Roman numerals by Schayes et al. [1967], appear between the temperatures of
70◦ C and 600◦C. The useful glow peaks for dosimetry are identified as III and III , and appear with different
luminosity for the samples of Fig. 19.18. Cameron et al. [1968] report that the integrated light yield from
peaks III and III comprise approximately 75% of the total light yield. Although there are some smaller glow

6 Studied and developed by Manufacture Belge des Lampes Électriques (or MBLE) in Belgium, these TLDs are no longer
manufactured.
Sec. 19.1. Luminescent Dosimeters 967

peaks at higher temperatures, they are generally not 


used for dosimetry because temperatures above 450◦ C  !
!
!"
can permanently damage CaF2 TLDs.  !!

The linearity of CaF2 is quite good, and these TLDs  



show good linearity for gamma-ray exposures up to 104
5 
R and exhibit only slight supralinearity up to 10 R.
CaF2 becomes sensitized at high gamma-ray exposures 

between 104 and 4 × 104 R, with a maximum gain in 

sensitivity ranging between 1.6 to 4 if annealed at 450◦ C 



for 30 minutes [Cameron et al. 1968; Sunta and Kathuria 

1971]. From Fig. 19.19, the main glow peak does shift

in temperature with increasing heating rate; however,      

the total peak area and the total peak height remain  

remarkably constant for a wide range of heating rates. Figure 19.18. Glow curves from several samples of natu-
Natural CaF2 is strongly sensitive to UV light, which ral CaF2 . Data were adopted and adjusted from those of
Schayes et al. [1967].
primarily affects the output of glow peak III . It is be-
lieved that UV irradiation assists with the movement of electrons from deep traps to shallow traps, producing
additional luminescence in glow peak III. Brooke and Schayes [1967] describe a method of UV sensitization,
or thermoluminescent build-up, that allows rereading of TLDs numerous times from a single radiation expo-
sure, provided that the initial exposure exceeds approximately 5 R. Overall, the overexposure of CaF2 :natural
causes a bleaching of the TLD and the signal changes from that of competing processes, including thermo-
luminescent build-up, charge transfer, and fading. TLDs unexposed to ionizing radiation tend to increase in
luminescence, while the radiation induced signals tend to decrease with UV exposure [Becker 1973].
CaF2 :Dy (TLD-200) Developed by Harshaw for commercial use,7 TLD-200 is a synthetic Dy-doped form of
CaF2 . It is highly sensitive, much more so than TLD-100, and thus can be used for low-dose measurements.
The glow curve is relatively complicated, as shown in Fig. 19.20, with two salient composite peaks, one glow
peak appearing between 80◦ C and 210◦ C and another high-temperature composite glow peak appearing
between 250◦C and 450◦ C [Yazici et al. 2002; Bidyasagar et al. 2014]. Each of these composite glow peaks is
formed from several trap levels, and their intensity changes with radiation type, dose, and preheat method.
TLD-200 is not as linear as CaF2 :MBLE or CaF2 :Mn, and begins showing peak height supralinearity
near a dose of 5 × 103 rad, extending up to approximately 5 × 104 rad before becoming sublinear [Hasan and
Charalambous 1983]. The integrated luminescence (all peaks between 50◦ C and 370◦ C) shows supralinearity
starting as low as 800 rad. Saturation occurs between an exposure of 105 R and 106 R [Becker 1973]. Becker
[1973] reports that linearity can be improved by pre-irradiation and annealing TLD-200 at 600◦C for two
hours.
Fading can be significant, reportedly up to 25% in a month if post-irradiation treatments are not applied
[Binder and Cameron 1969]. If illuminated during storage, for instance in a diffuse room light, fading can
increase up to 30% in a single day. The main cause of fading is from the low temperature glow peak
components. If eliminated by post-irradiation annealing, nominally 80◦ C for 10 minutes, the fading can
be reduced to 13% per month [Binder and Cameron 1969], but at the expense of 20%-30% reduction in
sensitivity.
CaF2 :Tm (TLD-300) Thulium-doped CaF2 was introduced as a dosimeter material in 1977 [Lucas and
Kapsar 1977] and put into commercial use as TLD-300 by Harshaw. The glow curve of TLD-300 (see
Fig. 19.21) displays two main composite peaks in the spectrum, centered near 175◦ C and 260◦ C, generally

7 Now produced by Thermo-Fisher Scientific. See Thermo-Fisher [2016].


968 Luminescent, Film, and Cryogenic Detectors Chap. 19




 

   





  !
 




    
 
Figure 19.19. Comparative results for natural CaF2 ,
showing deviation in peak height and area as a function Figure 19.20. Normalized glow curves for typical TLD-
of heating rate. The gamma-ray exposure was adjusted to 200 exposure measurements after gamma-ray irradiation.
be proportional to 1/RT for the peak height, while the ex- Data adopted and adjusted from those of Yazici et al. [2002]
posure was normalized for the peak area data. Also shown and Massillon-JL et al. [2008].
is the change in peak temperature with heating rate. Data
are from Gorbics et al. [1969].

labeled as peak 3 and peak 5, although the observed peak 5 is really a combination of peaks 5 and 6
[Massilon-JL et al. 2008]. A third glow peak is present if readout occurs within 24 hours of exposure and is
centered near 100◦ C; however, this glow peak usually fades after 24 hours and usually does not appear in
the glow curve. The output characteristics of TLD-300 are relatively stable and appear not to be affected
by the heating rate [Kafadar et al. 2013].
The luminosity of the two main peaks is strongly dependent on the linear energy transfer and the ratio
of peak 3 to peak 5 decreases with increasing LET. This feature can be used in dose interpretation in mixed
radiation fields. Furretta and Tuyn [1985] show that the ratio of peak 3 to peak 5 increases from 1.22 for
3
H beta-particle emissions up to 3.15 for 90 Sr beta-particle emissions. Because the ratio also shows a strong
dependence with heavy ions, Massilon-JL et al. [2008] suggest its use as an indicator of ion beam quality.
The recommended anneal process for TLD-300 is one hour at 400◦ C followed by a rapid quench cooling
in air to room temperature at a rate of 75◦ C per minute [Massillon-JL et al. 2008]. Fading is reduced to
approximately 5% over a 4-week period for both peak 3 and peak 5, while the contribution from peak 6
appears unaffected [Kafadar et al. 2013].
CaF2 :Mn (TLD-400) Mn-doped CaF2 was developed for thermoluminescent dosimetry at the Naval Re-
search Laboratory in the late 1950s and early 1960s [Ginther and Kirk 1957, Schulman et al. 1960]. The
general method of producing TLD-400 material is by first chemically precipitating CaF2 and MnF2 into
solution, following by filtering and drying the residue in an inert atmosphere. The sintered material is then
ground to particle sizes of about 100 microns and thoroughly mixed. Afterwards, the material is formed into
various shapes and sizes and sintered.
TLD-400 has a simple glow curve consisting of just one main glow peak appearing between 260 to 320

C, depending on the heating rate as shown in Fig. 19.22. The relatively higher glow peak temperature
indicates emission from a deep trap, yet CaF2 :Mn has high fading rate of up to 10% per month. TLD-400
has a higher intrinsic sensitivity than TLD-100, and can be used to measure radiation exposures below 1
mR. The response of TLD-400 is linear over a wide range, up to 3 × 105 R before sublinearity is observed
(See Fig. 19.12). Further, there appears to be no dependence on the type of ionizing radiation or LET as
observed with LiF-based TLDs. The dose rate dependence is relatively constant up to a heating rate of
Sec. 19.1. Luminescent Dosimeters 969



  







 
 


       
 
Figure 19.22. Comparative results for CaF2 :Mn dosime-
ters, showing deviation in peak height and area as a func-
Figure 19.21. Normalized glow curves for typical TLD-
tion of heating rate. The gamma-ray exposure was ad-
300 exposure measurements after gamma-ray irradiation.
justed to be proportional to 1/RT for the peak height, while
Data adopted and adjusted from those of Yazici et al. [2002]
the exposure was normalized for the peak area data. Also
and Massillon-JL et al. [2008].
shown is the change in peak temperature with heating rate.
Data are from Gorbics et al. [1969].

approximately 30◦ C per minute before both the relative glow curve peak height and integrated area begin
to decline. As with all CaF2 TLDs, TLD-400 is overly sensitive to gamma-ray energies below 100 keV.
Although filters can be used to soften the response to lower energy gamma rays and x rays, the same filters
can also over-attenuate soft x rays, thereby producing a lower measured dose.

Calcium Sulphate
Calcium sulphate (CaSO4 ) is a relatively high Z material that has been studied for use as a thermolumi-
nescent dosimeter. Mn-doped CaSO4 has a low temperature glow curve peak (see Fig. 19.23), which fades
rapidly at room temperature. Fading is reportedly to be as high as 40% within one day, and up to 85%
after three days [Fowler and Attix 1966]. Consequently, CaSO4 :Mn is not useful as a dosimeter except,
perhaps, for short-term laboratory experiments in which the TLD is read soon after irradiation. Regardless
of this drawback, CaSO4 :Mn is very sensitive to ionizing radiation and capable of measuring exposures in
the μR range [Fowler and Attix 1966]. The main reason for this perceived higher sensitivity is actually a
fortuitous benefit of the low-temperature glow curve, in which the background IR emissions from the heater
and TLD are small by comparison to the thermoluminescence. Hence, the signal-to-noise ratio is high so
that measurement of low doses is possible. The emission spectrum from CaSO4 :Mn peaks near 500 nm,
which is somewhat long in wavelength to be a good match to most bi-alkali PMTs. All forms of CaSO4 are
overly sensitive to gamma rays below 100 keV, much like CaF2 . Although the glow peak maximum shifts
from approximately 80◦ C to over 120◦C for heating rates between 10 C◦ /min up to 500 C◦ /min, the peak
height and peak area remain remarkably constant for heating rates below 150 C◦ /min (see Fig. 19.24).
Because of the high fading, other phosphors for CaSO4 were studied. For instance, Sm was tested as
an activator with encouraging results [Cameron et al. 1968], but the main glow peaks appear at 100◦C and
400◦ C, with an emission spectrum centered at 600 nm, too high for efficient coupling to conventional PMTs.
Of the activators explored, both Dy-doped and Tm-doped have proven to be relatively successful. The
main glow peak for both CaSO4 :Dy (also called TLD-900) and CaSO4 :Tm appears at approximately 225◦ C.
Although the glow peak appears simple, Souza et al. [1993] report at least ten peaks in the TLD-900 glow
curve, although only seven actually comprise the main glow peak. Of these deconvolved peaks Harvey et al.
[2010] note that only two or three are important for doses below 10 R.
970 Luminescent, Film, and Cryogenic Detectors Chap. 19

  !"
 !

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Figure 19.23. Normalized glow curves for typical Figure 19.24. Comparative results for CaSO4 :Mn
CaSO4 :Mn, CaSO4 :Tm, and CaSO4 :Dy (TLD-900) for ex- dosimeters, showing deviation in peak height and area as a
posure measurements after gamma-ray irradiation. Data function of the heating rate. The gamma-ray exposure was
adopted and adjusted from those of Yamashita et al. [1971] adjusted to be proportional to 1/RT for the peak height,
and Ekdal et al. [2014]. while the exposure was normalized for the peak area data.
Also shown is the change in peak temperature with heating
rate. Data are from Gorbics et al. [1969].

The main luminescent emissions from TLD-900 appear near 480 nm and 570 nm. By comparison, the
luminescent emission maximum from CaSO4 :Tm is near 450 nm, a better match to traditional alkali metal
PMTs, although CaSO4 :Tm is less sensitive to ionizing radiation than TLD-900. The luminescent response
for TLD-900 is linear up to approximately 3 × 103 R. Supralinearity appears between 3 × 103 R and 104 R,
beyond which sublinear behavior appears [Becker 1973]. As with many TLDs, saturation is reached at 105
R.
TLD-900 is significantly more sensitive than TLD-100 by about a factor of 30, and low gamma-ray
doses below a mrad have been measured. Fading is minor, reportedly as low as 2% in the first month
and 6% over a five-month period when stored at room temperature [Becker 1973]. Similar results were
reported by Guelev et al. [1994], who observed approximately 5% fading over a six-month period. However,
Harvey et al. [2010] report a much higher degree of fading near 30% in one month, attributed to low
temperature glow peaks apparently not considered in the Guelev et al. [1994] study. The annealing procedure
is straightforward, requiring no more than a 15-minute soak at 400◦ C. Yamashita et al. [1971] report that
TLD-900 is significantly sensitive to thermal neutrons while CaSO4 :Tm is not and conclude that the use of
CaSO4 :Tm is preferred in a mixed radiation field because of the high response that TLD-900 has to thermal
neutrons.

Lithium Borate (Li2 B4 O7 :Mn)


Lithium borate (LBO) is mainly attractive as a thermoluminescent dosimeter because of it low Z components
and low mass density. As a result, the response is nearly flat from 10 keV to 10 MeV, as shown in Fig. 19.10.
Its low density is closer to bone and soft tissue than most other TLD materials, which helps to simplify
dose conversions. Li2 B4 O7 is water soluble and hygroscopic, unless mixed and processed with 0.25% SiO2
by weight, which seems to stabilize it [Becker 1973].
Mn is the best known activator for Li2 B4 O7 and is often named TLD-800 for short. The emission
spectrum maximum for TLD-800 is reportedly at 605 nm [Gorbics 1966], a relatively long wavelength for
most PMTs. This maximum can be shifted to shorter wavelengths by doping with Cu (or Ag). Li2 B4 O7 :Mn
has emission maximum near 352 nm [Tiwari et al. 2010]. TLD-800 has a linear response to gamma rays up
Sec. 19.1. Luminescent Dosimeters 971



!
!


   









     
 

Figure 19.25. Comparative results for Li2 B4 O7 :Mn Figure 19.26. Normalized glow curves for typical
dosimeters, showing deviation in peak height and area as Li2 B4 O7 :Mn exposure measurements after gamma-ray ir-
a function of heating rate. The gamma-ray exposure was radiation. Data adopted and adjusted from those of Ya-
adjusted to be proportional to 1/RT for the peak height, mashita et al. [1971] and Ekdal et al. [2014].
while the exposure was normalized for the peak area data.
Also shown is the change in peak temperature with heating
rate. Data are from Gorbics et al. [1969].

to 150 R, becomes supralinear between 150 R and 105 R, eventually saturating at ×105 R. TLD-800 has
lower sensitivity to gamma rays than LiF, generally ten times less sensitivity than TLD-100. West et al.
[1967] report that TLD-800 sensitizes when irradiated with 105 R gamma rays and annealed for 15 minutes
at 300◦ C (see Fig. 19.13), achieving approximately 4 times the sensitivity for gamma-ray doses below 200
R. Becker [1973] reports that annealing is simple, requiring only a 15-minute soak at 300◦ C.
Gorbics et al. [1969] report that the peak height and peak area are relatively constant over a wide range
of heating rates; however, this result is markedly different from that reported by Kafadar et al. [2014], who
report large changes in peak area for TLD-800 when heated at rates above 120◦C/min. Both Gorbics et al.
[1969] and Kafadar et al. [2014] report glow peak temperature changes from below 170◦ C to nearly 220◦ C
over heating rates ranging between 10◦ C/min to 500◦C/min as shown in Fig. 19.25. Two glow peaks are
prevalent shortly after irradiation for both TLD-800 and Li2 B4 O7 :Cu. TLD-800 has one glow peak appearing
at approximately 100◦ C and the other at approximately 225◦ C (see Fig. 19.26). Li2 B4 O7 :Cu has a lower
temperature glow peak near 120◦ C, and also has a higher temperature peak reported as 205◦ C by Takenaga
et al. [1980], but reported as much higher at approximately 240◦ C by Aydin et al. [2013]. For all cases the
lower temperature glow peak fades rapidly, usually disappearing within a day [Schulman et al. 1967; Aydin
et al. 2013]. The higher temperature peak for TLD-800 fades by approximately 8% over a 30-day period
[Cameron et al. 1968], but there are differing fading results reported for Li2 B4 O7 :Cu. Wall [1982] reports
rapid fading for Li2 B4 O7 that was doped with Cu or co-doped with Cu and Ag. However, Aydin et al.
[2013] reports fading is approximately the same as TLD-800, fading about 10% over a 40-day period. Most
likely the preparation method is responsible for these differences, as demonstrated by Christenson [1967]
who increased the dosimetric response and range of TLD-800 by changing the preparation method.
Because of the constituent elements B and Li, the thermal neutron response of TLD-800 is relatively
high [Gambarini 2003], higher than TLD-100, but less than TLD-600 and TLD-900. Sunta et al. [1972]
report that the fast neutron response (from recoil protons) to gamma-ray response ratio was nearly 3 while
TLD-100 and TLD-900 response ratios were much less at 1.24 and 1.6, respectively.
972 Luminescent, Film, and Cryogenic Detectors Chap. 19

Beryllium Oxide (BeO)


Another low density thermoluminescent material is BeO, generally regarded as a “tissue equivalent” material.
The often quoted effective Z (or Zeff ) is 7.12.8 BeO is toxic in powdered form, but not as a ceramic, and
comes in three main forms, namely hot pressed (HP), slip cast (SC), and nuclear quality (NQ) [Scarpa 1970].
These three forms have different densities, with SC at 2.2 g cm−3 and the other forms approaching 2.8 g
cm−3 . It is relatively chemically inert and resistant to mechanical shock.
The glow curve spectra and the peak temperatures were observed to shift according to TLD manufacturing
process [Scarpa 1970]. Three different emission spectra were observed by Scarpa [1970] with peaks centered
differently at 210◦ C, 240◦ C, and 290◦C for SC, NQ, and HP BeO, respectively (see Fig. 19.27). The response
to gamma rays is fairly linear from 10 mR up to approximately 100 R, beyond which the output becomes
supralinear (see Fig. 19.12). Although HP BeO showed up to 20% fading in three days, the other forms
demonstrated approximately 4% fading within 24 hours with no significant fading thereafter.
Measurements conducted by Crase and Gammage [1975] indicate that various forms of BeO all produce
spectra in the UV region, generally between 200 nm to 400 nm with a peak near 265 nm. Consequently,
most commercial PMTs are insensitive to much of the spectrum, and special PMTs (or TL readers) with
deep UV sensitivity must be used (see Sec. 14.1.2 for more information on PMT windows).
BeO is more sensitive to gamma rays than Li2 B4 O7 , but much less so than LiF by about a factor of 3
[Shani 1991]. The sensitivity of SC BeO is practically linear for gamma-ray energies ranging from less than 20
keV to over 1 MeV, while the other forms are slightly higher in response for energies below 500 keV [Scarpa
1970]. Although linear at low doses, competition from non-radiation induced emissions from pyroelectric
incandescensce contribute to background, making it difficult for accurate low-dose measurements. Exposure
to light can depopulate BeO traps, inducing fading. Consequently, BeO TLDs should be handled carefully
and not exposed to light during exposure or readout.
Aluminum Oxide (Al2 O3 )
Aluminum oxide is the chemical name for a mineral often regarded as a precious gem. If it has a small
amount of Cr impurity (Cr2 O3 ) it is called ruby. Other gem quality samples are called sapphires, associated
with a wide range of colors according to the residual impurities. Otherwise, the common name for Al2 O3 is
corundum. Aluminum oxide is one of the hardest known substances, rated as 9 on the Mohs hardness scale.
Aluminum oxide is mostly chemically inert and it is water insoluble. It has high electrical resistance and its
melting point is extremely high at 2072◦C.
Aluminum oxide was first studied for its thermoluminescent properties by Rieke and Daniels [1957], and
later as a dosimeter by McDougall and Rudin [1970]. Samples with Cr contamination (ruby) produced a
glow curve peak between 350◦ C and 400◦C with a maximum emission wavelength near 650 and 700 nm.
Unfortunately, at such high temperatures infrared emissions contaminate the luminescent emissions, and the
emission wavelength is well beyond the sensitivity range of most photomultiplier tubes.
Pure Al2 O3 has a thermoluminescent glow peak wavelength near 410 nm. Portal et al. [1980] report
several glow peaks for Al2 O3 with 0.7% Na and 4% Ti, appearing at approximately 140◦ C, 265◦ C, 450◦ C,
and 630◦ C. See Fig. 19.28 for example glow curves. The lowest temperature glow peak fades quickly, while
the higher two glow peaks have IR contamination during readout. It is the peak at 265◦ that has importance

8 Forthe purpose of gamma-ray attenuation through a compound material, a fictitious Zeff is often used. This number is often
determined by the empirical relation [Murty 1965]

N
(Zeff )2.94 = fi Zi2.94 ,
i=1
where fi is the fraction of electrons associated with element i having atomic number Zi . Although often used, the reader is
cautioned that this is an empirical expression, and the exponent of 2.94 may not be accurate. In fact, Murty [1965] states in
his publication that measurements indicate that 3.1 instead of 2.94 for the exponent yields improved results.
Sec. 19.1. Luminescent Dosimeters 973

 
#
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Figure 19.28. Normalized glow curves for typical Al2 O3
Figure 19.27. Normalized glow curves for typical BeO measurements after gamma-ray irradiation. Data are
exposure measurements after gamma-ray irradiation. Data adopted and adjusted from those of Portal et al. [1980]
are adopted and adjusted from Scarpa [1970]. and Kortov and Ustyantsev [2013].

in dosimetry. The effective Z is 10.2, and below 200 keV Al2 O3 has higher sensitivity than TLD-100, but
less so than CaF2 (Fig. 19.10).
When doped with carbon, Al2 O3 has relatively good thermal stability, and is often denoted as TLD-
500. The peak emission wavelength is 420 nm, well matched to the response function of common PMTs.
Further, the thermal fading is approximately 3% per year and the dosimetric sensitivity can be as low as
5 μR. Kortov and Ustyantsev [2013] report multiple different glow curves dependent on the dose level. For
instance, a single salient glow peak appears near 185◦C at a dose of 800 mR from 60 Co, shifting downward to
165◦ C at a dose of 106 R. Several high temperature glow peaks appear for doses above 3 × 106 R, the main
one appearing near 425◦C. Although Al2 O3 :C functions as a thermoluminescent material, Akselrod et al.
[1998] note that thermal quenching changes luminosity with heating rate. Consequently, because optically
stimulated luminescence (OSL) demonstrates increased sensitivity and also the lack of thermal quenching,
TLD-500 has instead gained popularity as an OSL dosimeter.

19.1.2 Optically Stimulated Luminescent Dosimeters


Closely related to thermally stimulated luminescence is optically stimulated luminescence (OSL) [McKeever
2001], with the main difference being in the method used to induce photon emissions. Both an OSLD and
a TLD use a ceramic material in which intrinsic or activated traps store charge produced from radiation
absorption events. However, instead of using thermal methods to release electrons from traps and into
luminescent centers, energetic photons of sufficient energy are used to accomplish this task. Because the
OSLD is not heated, problems with thermal destruction of the dosimeter are nearly eliminated. Further,
select portions of the dosimeter can be sampled with a focused UV laser, a feature not possible with the
uniform heating used in thermoluminescent dosimetry. Hence, an OSLD may have only a portion of the
sample area illuminated, leaving other areas of the dosimeter unaltered for later measurements if required.
TLDs produce a glow curve that corresponds to light emissions from increasing trap energies as a function
of increasing temperature. As temperature is increased, definitive features in the glow curve appear in the
output spectrum. However, OSL dosimeters are illuminated with a light source that can affect shallow
and deep traps simultaneously. This illumination is usually in the form of focused laser light. The output
response, i.e., the emitted light, depends on several characteristics of the input illumination such as the
wavelength, light intensity or power, and transient nature of the illumination.
974 Luminescent, Film, and Cryogenic Detectors Chap. 19

Because of the similarities between TL and OSL dosimetry, Fig. 19.1 adequately depicts the initial
process of radiation absorption. However, the stimulated emission process is quite different, as illustrated in
Fig. 19.29. Instead of heat, energetic photons of energy greater than or equal to the trap energies are used
to depopulate the dosimeter traps. The ejected electrons can then fall into luminescent centers accompanied
by photon emissions, or the electrons may instead fall back into traps. However, if the electrons fall back
into traps, they can subsequently be re-emitted by the optical stimulation, and can still contribute to the
output signal if they fall into a luminescent center. To obtain a useful output signal, it is important that the
stimulation wavelength be longer than the emission wavelengths, thereby facilitating filtering and reducing
induced emissions unrelated to the radiation dose. For instance, the most commonly used commercial OSL
dosimeter is Al2 O3 :C, which emits a broad wavelength spectrum centered at 420 nm (violet-blue). However,
the stimulation wavelength is larger, optimized at 525 nm (green light). In this manner the stimulated
luminescence can be separated from the interrogation light.
Modeling the Stimulated Emission
a
shallow traps fade or
Electrons in an excited state can go to a lower energy
contribute to luminescence
state with or without photon emission with probabilities
1 2 3 4 pr and pnr , respectively. Recall from the configuration
EC coordinate diagram of Fig. 13.2, there is a probability
pnr that an electron in an excited state can move directly
to the ground state at the crossover D → D without any
emission stimulated
by light photon emission. This probability is described by
hn pnr = p0 e−ΔE/kT , (19.24)
where ΔE is the activation energy required to move an
EV
electron from the bottom of the conduction band C to
Figure 19.29. Band diagram depicting detrapping and reach the crossing point at DD in Fig. 13.2 and p0 is
emission during the stimulation time. The shallow traps a scaling constant referred to as the frequency factor.
(1) fade or can contribute partially to the OSL. Dosimeters The radiative transition probability pr is unaffected by
traps, (2 and 3) contribute to the dosimetry measurements.
With adequately energetic optical stimulation, deep traps temperature.
(4) can also contribute to the dosimetry signal. Also, re- The optical luminescent efficiency is defined as
trapping can occur at all trap states (2,3,4), yet they can pr τnr
also be simultaneously optically excited, thereby continue η= = , (19.25)
to provide dosimetry information. pr + pnr τr + τnr
where τr = 1/pr is the mean radiative lifetime and τnr = 1/pnr is the mean non-radiative lifetime. Substi-
tution of Eq. (19.24) into this definition gives
pr 1
η= = , (19.26)
pr + p0 e−ΔE/kT 1 + ce−ΔE/kT
where c = p0 /pr = p0 τr , a constant.
From Eq. (19.26), it is readily apparent that as the temperature of the OSL material increases, the
luminescent efficiency should decrease. The loss of luminescence with temperature is referred to as thermal
quenching. The total lifetime of excited charges is also a function of the radiative and non-radiative transition
probabilities, namely
τr τnr τr
τ (T ) = = . (19.27)
τr + τnr 1 + τr p0 e−ΔE/kT
From this result it is seen that the total lifetime also decreases as the temperature increases. Akselrod et al.
[1998] show that a plot of τ versus temperature can yield both the values of the frequency factor p0 and the
activation energy ΔE.
Sec. 19.1. Luminescent Dosimeters 975

The use of OSL as a dosimetry technique was first explored by Huntley et al. [1985] as a method to date
geological samples. The test samples were natural quartz irradiated with 514.5 nm light. The technique
was developed over several years for geology, and years later was recognized as a potential technique that
can be used for radiation dosimetry [Bøtter-Jensen and McKeever 1996]. Numerous materials have been
investigated for use as OSL dosimeters, including many traditional TLD materials. The most successful, and
most popular, is carbon activated alumina, Al2 O3 :C.
For constant illumination, the rate of stimulation from a trap, with units s−1 , for photons of energy Eph
is given by
1
Rte = σt φph = , (19.28)
τd
where τd is the decay constant, σt is the photoionization cross section, and φph is the photon flux of energy
Eph [Bøtter-Jensen et al. 2003]. For simplicity, suppose all electron traps are at the same energy level and
all luminescence centers, likewise, are at a single lower energy level. Because there is no charge on the
material (the charge neutrality condition), the concentration n of electrons in the conduction band and the
concentration Nte of electrons in traps must equal the concentration p of holes in the valence band and the
concentration Nrh of holes stored in recombination centers. After the OSLD has been exposed to radiation,
the free electrons and holes either fall into traps or recombine so that n = p = 0. Here it is assumed that
there is a wide band gap with negligible thermal generation of free charges and that the stimulation photons
have insufficient energy to excite electrons from the valence band to the conduction band.
However, upon illumination this equilibrium balance is altered. The rate of gain of electrons in the
conduction band equals the rate at which electrons leave their traps plus the rate at which electrons fall
from the conduction band into recombination centers, i.e.,

dn(t) dNte (t) dNrh (t)


=− + . (19.29)
dt dt dt
The rate of increase in the density of trapped electrons equals the rate per unit volume that electrons are
excited out of the traps (negative change) plus the rate per unit volume that free electrons fall into the traps,
namely
dNte (t) Nte (t) Nt − Nte (t)
= −Rte Nt + pec n(t)Nt , (19.30)
dt Nt Nt
where pec is the free electron capture probability per unit time, Nt is the trap concentration and (Nt −Nte )/Nt
is the fraction of traps that are empty and able to receive an electron. The rate of decrease in the hole
concentration at recombination centers is the rate at which electrons from the conduction band fall into
open recombination centers, i.e.,
dNrh (t) Nrh (t)
= −per Nr n(t), (19.31)
dt Nr
where per is the probability, per unit time, of an electron in the conduction band recombining with a hole
at a recombination center, which has a concentration of Nr , and Nrh /Nr is the fraction of recombination
centers which contain a hole and are able to receive an electron from the conduction band.
To obtain an expression for the intensity of the stimulated luminescence beginning at t = 0, two simpli-
fying assumptions are made. First, it is assumed that the probability of exciting an electron out of a trap
and falling into a recombination center is much higher than that of a free electron returning to a trap center.
Hence Eq. (19.30) is simplified to
dNte (t)
= −σt φph Nte (t), (19.32)
dt
976 Luminescent, Film, and Cryogenic Detectors Chap. 19

whose solution is
0
Nte (t) = Nte exp[−σt Φph t], (19.33)
0
where Nte is the trap-filled population at t = 0. The second assumption is that the change in recombination
center population equals the change in trap population, i.e., dn/dt ≈ 0. Thus, from Eq. (19.29) the stimulated
luminescence can be described by
dNrh (t) dNte (t)
I = −C = −C . (19.34)
dt dt
where C is a constant to account for the size of the interrogation volume and the luminescence efficiency. For
a constant optical stimulation for t ≥ 0 with a constant photon flux of energy Eph , the luminescent intensity
is found by substitution of Eqs. (19.32) and (19.33) into Eq. (19.34) to give
0
I = CNte σt φph exp[−σt φph t], t > 0, (19.35)
0
where Nte is the trap-filled population at t = 0. Constant power illumination is referred to as CW-OSL
(continuous wave OSL) in which the OSL dosimeter is illuminated with a selected bandwidth of wavelengths
at constant power for a specific time. Electrons depopulate the storage traps, fall into recombination centers,
and produce luminescence. Under CW operation, Eq. (19.35) indicates that the expected luminescent output
is a rapidly decaying exponential function of time. This behavior is expected because light emissions decrease
with time as the traps are depopulated. These trap emissions are concurrent. Spectral emissions develop
simultaneously according to the trap emission probability.
The integrated luminescence Ilum over time period t1 is
 t1 t1
0 −σt φph t 
 
Ilum = 0
CNte σt φph e−σt φph t dt = −CNte e  = CNte
0
1 − e−σt φph t1 . (19.36)
0 0

0
This result shows that the luminescent yield is proportional to the initial filled trap density Nte . If the initial
filled trap density is a linear function of radiation dose, then this integrated luminescence can be used to
measure the dose [Yukihara and McKeever 2008].
Multiple Traps for Electrons and Holes Because an OSL dosimeter usually has multiple trap energies
as well as several luminescent center energies, the output spectrum is, therefore, not a simple exponential
function of time. Instead it is superposition of emissions from multiple trap energies and luminescence of
different energies. Other factors that contribute to the spectral output are competing trapping centers,
thermally induced emission (usually from shallow traps), retrapping, and photo-excitation of electrons from
deep to shallower traps. In some circumstances, the combined output spectrum may be best modeled as an
inverse power function rather than as a simple exponential dependence [Yukihara et al. 2004].
The effect of shallow traps in an OSL dosimeter is to produce a concentration of competing traps that
initially reduces the luminescence. These shallow traps fade rapidly after irradiation and a large fraction of
the centers depopulate before optical stimulation. Consequently, these empty traps compete with luminescent
centers for electrons during the optical stimulation step, causing a reduction in the emitted luminosity. As
the intensity measurement continues, a steady-state condition is reached in which trapping at shallow traps
is matched by detrapping and results in an increase in luminosity. As the measurement continues further,
the luminosity characteristic eventually decreases with time, similar to the ideal case without shallow traps.
The effect of deep traps is similar to that observed with TLDs and causes an apparent increase in dose
sensitivity, or sensitization. Upon irradiation, a new and pristine OSL dosimeter has energetic electrons
excited across the band gap. Many of these electrons diffuse through the material and drop into traps,
including shallow, medium, and deep traps. In the present case, the medium level traps that participate
Sec. 19.1. Luminescent Dosimeters 977

  









 



 

    
  

Figure 19.30. Luminescent output from Al2 O3 :C OSLDs for three types of laser stimulation, (a) CW-OSL, (b) LM-OSL, and
(c) POSL. The OSLDs in (a) and (c) are Al2 O3 :C (LuxelTM ) and in (b) it is a Al2 O3 :C TLD-500. After Bøtter-Jensen et al.
[2003].

in the dosimetric signal are referred to as dosimetry traps. During optical stimulation, a large percentage
of shallow and dosimetry traps are emptied, but the deep traps are not. As these deep traps are filled,
and remain filled, they are eliminated as competing traps. Consequently, subsequent irradiation of an OSL
produces a higher percentage of filled dosimetry traps because there are fewer competing deep traps. The
end result is higher luminosity per unit dose during optical stimulation.
The excitation wavelength is selected to correspond to sub-bandgap energies. The purpose for this choice
is simple; the stimulation process is responsible for exciting more electrons into dosimetry traps. However,
it is still possible for photons during the optical stimulation process to excite electrons across competitive
traps. For instance, electrons in deep traps may be transferred to dosimetry traps.
OSL Systems
OSL readers have at least two main components, namely, a light source to stimulate the dosimeter and a
photosensitive receptor to detect the stimulated luminescence. A challenge for these components is the vast
difference in luminescent intensity between the light stimulation source and the luminescent emissions, a
difference that can span over 14 orders of magnitude ranging between 1016 photons cm−2 s−1 for stimulation
and 102 photons cm−2 s−1 for low dose luminescence [Yukihara and McKeever 2011]. OSL systems are
designed to reduce photo-ionization and photo-transference of electrons. A long-pass filter9 is placed between
the light source (usually a laser, photodiode, or lamp) and the OSL dosimeter. Another filter is also placed
between the OSL dosimeter and the light collection device (typically a PMT), usually a bandpass filter
which transmits photons with wavelengths between 290 nm to 370 nm [Yukihara and McKeever 2008].
The bandpass filter reduces scattered light from the light source from entering the PMT, while passing the
prominent wavelengths from optically stimulated luminescence. Additional components may include optical
components, such as mirrors and lenses, to guide and focus the light, both stimulated and luminescent.
There are at least three types of stimulation systems in use for OSL, listed as continuous wave (CW-OSL),
linear modulation (LM-OSL), and pulsed (POSL). These systems are briefly described here but more detailed
descriptions can be found in the literature [Bøtter-Jensen et al. 2003; Yukihara and McKeever 2011].
CW-OSL The CW system focuses light of constant power onto an OSL dosimeter in a step input, as
depicted in Fig. 19.30(a). CW-OSL remains the most popular method to sample an OSL dosimeter, mainly
because of its simplicity and reliability. The output response is described by Eq. (19.35) in which the
expected output signal is largely modeled as an exponentially decreasing function. The output signal is
0
mainly a function of the initial trap filled density Nte , the stimulation intensity φph , and the time duration
of the stimulation t. For a fixed illumination time period t1 = Δt with constant power φph , the integrated

9 These filters are used to filter short wavelengths that may excite electrons across a bandgap or produce prominent photo-
transference while at the same time passing longer wavelengths that still can excite electrons out of dosimetry traps.
978 Luminescent, Film, and Cryogenic Detectors Chap. 19

intensity produces a luminescent output proportional to the initial trap-filled population. A sample taken
over a short time period, 1 second for instance, is sufficient to gain the required information on dose. After
such a short sampling time, many of the trap states may remain filled. The OSL can then be stored and
re-read if so required, taking into account the time period of the prior optical stimulation.
Notably, integration of Eq. (19.35) for the total luminescence Itot , i.e., Δt → ∞, is solely a function of
0
the initial number of filled traps Nte , namely
 ∞
Itot = C 0
Nte σt φph e−σt φph t dt = CNte (t0 ). (19.37)
0

Consequently, the intensity of the stimulation light φph does not affect the total luminescence or resulting
measured dose. Hence, the light stability and intensity of the stimulation source have, theoretically, no
effect on the measured output or dose provided that the volume of the OSL dosimeter is cleared of all
trapped electrons by this long-term stimulation. However, the initial luminescence I(t = 0+ ) emitted by
the stimulated OSL dosimeters is in fact a function of the intensity φph of the light source, as shown in
Eq. (19.35), and the total light output for a finite Δt is, from Eq. (19.36), also a function of φph . Hence, if
the user reads only part of the OSL dosimeter traps during a measurement, it is important that the light
source be stable during the measurement time to obtain reliable results.
The simple model of Eq. (19.36) does not take into account the possibility of different trap energies
participating in the luminescent output. Further, it does not consider retrapping of charges, effectively
prolonging the stimulated luminescence. Curve fitting indicates that a power function may in fact describe
better the luminescent behavior of a real OSLD than does a simple exponential.

POSL Although filters are used to reduce contamination from scattered light from the source, these same
filters can also absorb some of the optically stimulated light. If there is significant overlap between the
stimulation spectrum and the OSL spectrum, then part of the OSL signal is sacrificed to eliminate scattered
light from the laser source. Because the intensity of the stimulation light is orders of magnitude greater than
the OSL output, the stimulation light leakage that arrives at the light sensor may still have an intensity
comparable to that of the optically stimulated luminescent light reaching the sensor.
Pulsed mode systems were developed as a readout system that can reduce scattered light from contami-
nating the OSL signal. The technique involves the use of a pulsed laser to stimulate luminescence from the
OSL dosimeter, while measuring the luminescence between pulses [McKeever et al. 1996]. Such a system
still has filters to reduce the detection of scattering photons. However, between pulses, the counting system
is gated such that current from the PMT is measured only while the laser is off. During the pulse, the elec-
trons in traps are elevated to the conduction band and can drop into luminescent centers. When the light
is switched off, these free electrons continue to fall back into luminescent centers and traps, hence continue
to produce luminescence. If the concentration of electrons in excited luminescent centers, before decay and

photon emission, is Nre , the process can be modeled as

dNre (t) N ∗ (t) dNte (t)
= − re − , (19.38)
dt τd dt

where the change in the excited luminescent center population is equal to decay of the luminescent centers
with time constant τd plus the decrease of trapped electrons into luminescent centers. Substitution of
Eq. (19.32) and Eq. (19.33) into Eq. (19.38) gives
∗ ∗
dNre (t) Nre (t)
+ = Rte Nte (t) = Nte (0)Rte exp[−Rte t], (19.39)
dt τd
Sec. 19.1. Luminescent Dosimeters 979

where the stimulation rate Rte = σt φph has units s−1 . The solution of this differential equation is

∗ Nte (0)Rte τd
Nre (t) = A exp[−t/τd ] + exp[−Rte t], (19.40)
1 − Rte τd
where A is a constant defined by an initial condition.
Now apply this result to the POSL chain of laser pulses shown in Fig. 19.31. Suppose that at the

beginning of a pulse at time tb , the concentration Nre (tb ) of luminescence centers is known. Then from
Eq. (19.40) the constant A is found to be

∗ Nte (0)Rte τd
A = etb /τd Nre (tb ) − exp[−Rte tb ] . (19.41)
1 − Rte τd

Substitution of A into Eq. (19.40) gives for t ≥ tb

∗ ∗ Nte (tb )Rte τd E −Rte (t−tb ) F


Nre (t) = Nre (tb )e−(t−tb )/τd + e − e−(t−tb )/τd , (19.42)
1 − Rte τd
where Nte (tb ) = Nte (0) exp[−Rte tb ]. The decay of the excited luminescent center, and the emitted lumines-

cent intensity, during a laser pulse, is I(t) = CNte (t)/τd or


Nte (tb ) (tb −t)/τd Nte (tb )Rte τd Rte (tb −t)
I(t)/C = e + (e − e(tb −t)/τd ), tb ≤ t ≤ te
τd τd (1 − Rte τd )

where tb = (m − 1)(tp + Δt), m = 1, 2, . . . , M. (19.43)

Here Δt is the time duration between pulses and tp is the optical pulse width. Between pulses, there is no
optical stimulation (Rte → 0), and the emitted luminescent intensity is

Nte (te ) (te −t)/τd
I(t)/C = e , where te = tb + tp = (m − 1)Δt + mtp . (19.44)
τd
During the stimulation time tp = te − tb , it is usual to close the electronic gate on the PMT signal, thereby
avoiding the inclusion of scattered light. Consequently only the light emitted during the time period between
pulses Δt is measured. Examples of the emitted luminescence are shown in Fig. 19.31.
Consider the light emitted during Δt to that over a single period (tp + Δt). For a constant measure-
ment/period ratio, the ratio of measured light to the total luminescence increases with frequency. If the
stimulation time is relatively long, followed by decay, a large fraction of light is lost during stimulation, with
the luminescence decaying to low values. In the example of Fig. 19.31(left), the amount of light emitted
after a stimulation pulse is approximately 40% for a frequency of 6.67 Hz. Because the optical signal is not
measured during stimulation, this result means that 60% of the signal is lost. By increasing the frequency,
the ratio of lost luminescence decreases. From the example of Fig. 19.31(b), with all parameters the same
except that the frequency is increased a hundredfold to 667 Hz, the percentage of measured light increases
to approximately 80%. Although Fig. 19.31 serves to demonstrate the general trend for POSL, the duty
cycle10 in the example is only 33.3%. In practice, the duty cycle is often shorter and on the order of 10%.
The ratio of lost luminescence decreases as the decay constant τd increases. To improve the measurements,
it is best to select a stimulation pulse width tp equal to or less than the luminescence decay constant τd .

10 The fraction of a period that the stimulation source is active.


980 Luminescent, Film, and Cryogenic Detectors Chap. 19

   

 
 
   

   
 
 
 

   

 
 
 
 
 

 
             
   

Figure 19.31. POSL luminescence signal with the stimulation pulse width equal to 1/3 of the total period. The gray region
indicates the time tp when the laser pulse is activated and the output signal is switched off, and the clear area represents the
time period Δt when the luminescence is measured. On the left, the period is 150 ms (6.67 Hz) with tp = 50 ms and on the
right the period is 1.5 ms (667 Hz) with tp = 500 μs. All other parameters are the same.

For a given value of τd , the pulse frequency and pulse width tp can be adjusted to optimize the light yield
while reducing contamination from scattered light. The general luminescent trend for a POSL measurement
is shown in Fig. 19.30(c) where it is seen that the luminescence initially increases, and begins to decrease as
the filled traps depopulate. At the end of the measurement, when the laser is switched off after a series of
pulses, the remaining excited luminescent centers decay away.
LM-OSL Linear modulation is an optical stimulation method in which the optical intensity is linearly
increased over time so that the stimulation rate (s−1 ) of removing a trapped electron is
t
, Rte (t) = σt φmax (19.45)
T
where φmax is the maximum optical power and T is the stimulation time period which begins at t = 0. The
luminescent decay time constant is now a function of time
1 T
τd (t) = = . (19.46)
Rte σt φmax
The trapped electron concentration is given by
dNte (t)
= −Rte (t)Nte (t), (19.47)
dt
whose solution is
σt φmax t2
Nte (t) = Nte (0) exp − . (19.48)
2T
The optical luminescence produced is thus
dNte (t) t −σt φmax t2
I(t) = −C = CNte (0)σt φmax exp . (19.49)
dt T 2T
The intensity maxima is easily found to be,
<
T
tmax = . (19.50)
σt φmax
Sec. 19.1. Luminescent Dosimeters 981

Substitution of Eq. (19.50) into Eq. (19.49) yields the maximum luminescence

σt φmax 1
Imax = Nte (0) exp − . (19.51)
T 2

The general luminescent shape is shown in Fig. 19.30(b), where it is seen that the luminescence increases
from zero to a maxima and then decreases as the traps depopulate. It is these maxima features that Bular
[1996] argues as advantageous, especially in the presence of multiple traps. Unlike the CW-OSL method in
which multiple traps blend together to produce a single decay curve, each trap level shows a maxima with
the LM-OSL method, thereby making identification of the individual traps possible. Nonetheless, for the
same sample material, the total area under the luminescence curves are the same for CW-OSL and LM-OSL.
Although numerous groups have experimented with LM-OSL (see references in Yukihara and McKeever
[2011]), it has not yet received widespread acceptance. Complications arise from non-linear light increase
associated with the stimulation source, spectral shift of the stimulated luminescence as the power is increased,
and changes in background light leakage measured by the PMT as the light source power is increased.
OSL Materials
Materials for optical stimulation luminescence include a variety of synthesized and natural minerals. Many
of the synthesized materials can be used for radiation measurements, mainly because the storage traps and
luminescent centers can be controlled during synthesis. Of these synthetic materials, Al2 O3 :C is the most
popular for dosimetry. Many natural minerals that exhibit OSL characteristics can be used to determine
post-factum doses and are used for geological dating. A select few of these materials are described here.
Aluminum Oxide (Al2 O3 :C) Carbon activated aluminum oxide (Al2 O3 :C) was originally proposed
as a TLD, yet has gained popularity as an OSL dosimeter [McKeever and Akselrod 1999; Aksel-
rod and McKeever 1999]. Al2 O3 has a high sensitivity to low radiation doses, and is now in
wide-spread use as a commercial dosimeter, having replaced TLD materials for many applications.
Carbon doped alumina has a main emission line near 
420 nm with a decay constant of 35 ms, and a lesser
fast emission at 335 nm with a time constant less
 


than 7 ns. Both of these emissions are produced
by stimulation of the dosimeter traps with green 
light, optimized at 525 nm. Reported sensitivity
ranges from 1 mrem (10 μSv) up to 104 rem (100 
Sv); however, the uncertainly for low doses can be


greatly affected by the environmental background ra- 

diation [Gilvin and Perks 2010]. When stimulated


with CW-OSL, the maximum luminescence occurs 

with a stimulation wavelength near 500 nm as shown



in Fig. 19.32. Shown in Fig. 19.33 is a decay curve for       
90
Al2 O3 :C after a dose of 60 mGy from a Sr source.      
Room-temperature thermal fading is reportedly not
appreciable up to 85 days after irradiation. Bøtter- Figure 19.32. OSL luminosity versus the stimulation wave-
length for Al2 O3 :C. Data are from Bøtter-Jensen et al. [1997].
Jensen et al. [1997] report fading is approximately
only 1.8% after 27 days and, subsequently, becomes relatively stable [Schembri and Heijmen 2007].
Although the fast UV emission at 335 nm increases the total optical stimulated luminescence, it is the
longer wavelength emissions with maxima near 420 nm that are usually used for dosimetry. The 420 nm
emission is attributed to F-center luminescence [Yukihara and McKeever 2008]. Optical excitation from
982 Luminescent, Film, and Cryogenic Detectors Chap. 19

the dosimeter traps produces free electrons that recombine with F+ -centers. The inclusion of carbon in
the growth process enhances the formation of these F+ -centers by replacing a fraction of the trivalent Al3+
ions with C2+ ions [McKeever et al. 1999]. The cap-
 ture of an electron produces an excited F-center, and


these excited F-centers de-excite by releasing a pho-


ton. Dosimetric linearity of up 5 × 103 rad (50 Gy) has
been reported for the F-center emission from Al2 O3 :C
OSL dosimeters [Yukihara and McKeever 2006]. With-
out proper filtration, the contribution to the total signal
by the UV emission can be significant, approximately
20% of the F-center signal for low doses and increas-
ing to nearly the same as the F-center emission at high
doses. Bandpass filters designed to pass F-center emis-
sion wavelengths can be used to reduce the influence of
 the UV emission.

The CW-OSL responses (Fig. 19.34) reveal sensiti-
Figure 19.33. An OSL decay curve for Al2 O3 :C after zation (superlinearity) with both the initial intensity
irradiation with 60 mGy from a 90 Sr beta particle source. (measured within the first 3 seconds of stimulation) and
The OSL decay curve is for constant power stimulation
−2
(16 mW cm ) with wavelength band of 420 to 550 nm.
the total luminescence (integrated over 300 seconds of
Data are from Bøtter-Jensen et al. [1997]. stimulation). Experiments that remove the UV compo-
nent indicate that these emission centers are responsible
for the supralinearity observed for doses above 103 rad
(10 Gy). Because of the short time constant, the UV
component can be eliminated from the measurement by
using POSL. During the stimulation pulse, most of the
UV component is released and does not contaminate the
measurements between pulses. Sublinearity is observed
for doses above 104 rad (100 Gy) for both UV and F-
center emissions.
The dose response can be affected by the dose his-
tory as deep traps become filled over time and are not
emptied by annealing. An advantage of single crystal
Al2 O3 :C dosimeters over OSLD formed from powder on
Figure 19.34. OSL beta particle dose response from a tape is that crystals can be annealed at high tempera-
Al2 O3 :C single crystal and from a Luxel Al2 O3 :C tape. tures to remove electrons from deep traps, up to 900◦ C
Initial OSL response is for the first 3 seconds of optical [Bøtter-Jensen et al. 1997]. This annealing procedure en-
stimulation. Total OSL area is for the integrated response
over 300 seconds of optical stimulation. Data are from sures that background and sensitization from deep traps
Yukihara et al. [2004]. does not build up over time. However, much like TLDs,
the uniformity of the carbon doping determines the vari-
ability of response, and large variations can be present within and between batches. Hence, crystalline
Al2 O3 :C OSL dosimeters can have a large variance in luminescence among samples.
Just as with TLDs, commercial Al2 O3 :C OSL material can be pulverized after crystal growth and mixed
with multiple batches to improve uniformity amongst samples. The pulverized materials are bound with
plastic to produce a length of tape. This tape is then sliced into sections for commercial use as OSL
dosimeters. These OSL dosimeters cannot be annealed at high temperatures because the plastic binder is
destroyed. Although optical bleaching can be used to empty most of the dosimeter traps, it is not adequate
to empty the deepest traps. Consequently, the background luminescence increases with integrated dose.
Sec. 19.1. Luminescent Dosimeters 983

Drawbacks to the use of Al2 O3 :C OSL dosimeters include the high effective Z number and the presence of
shallow traps that makes the material sensitive to light. The effective Z number is 11.3, and the low energy
response to gamma rays can be quite high, comparable to SiO2 (see Fig. 19.10), so that Al2 O3 :C OSL
dosimeters overrespond to x rays and low-energy gamma rays. The shallow traps can affect the total light
output, but generally fade rapidly at room temperature. Edmund and Andersen [2007] report that shallow
traps in Al2 O3 :C can affect the luminescent yield. If the irradiation temperature cannot be maintained at a
constant temperature, they recommend a correction factor between -0.2% to 0.6% per ◦ C over a range from
10◦ C to 50◦ C.
Beryllium Oxide Beryllium oxide (BeO), or beryllia, is a thermoluminescent material and has been used
as an OSL dosimeter. The luminescent spectrum reported by Bular and Göksu [1998] has a broad spectrum,
ranging from 420 to 550 nm, with a maximum peak at 435 nm. Sommer et al. [2008] report the use of 455 nm
light to stimulate these emissions and a Schott DUG11X optical filter to make luminescence measurements.
BeO OSL dosimeters are linear over a wide range, extending from 100 μrad (1 μGy) [Sommer et al. 2007] up
to 1000 rad (10 Gy) [Bular and Göksu 1998]. Sub-linearity appears at approximately 2000 rad (20 Gy), and
the onset of saturation is evident at approximately 10 krad (100 Gy) [Sommer et al. 2008]. The low effective
Z of 7.14 makes these OSLDs almost “tissue equivalent” and they have a relatively flat response for low- to
high-energy gamma rays (see Fig. 19.10) with only a slight under-response to low-energy gamma rays.
Short-term fading from shallow traps amounts to approximately 6% loss within the first few hours of irra-
diation. The fading becomes almost negligible thereafter and is less than 1% over a 6-month period [Sommer
et al. 2007]. There is a temperature dependence on the decay constant τd of the main luminescent centers,
ranging from 27 μs at room temperature down to 800 ns at 140◦C [Yukihara and McKeever 2011]. This
decrease in decay time constant is largely due to non-radiative transitions. Also, the luminescent efficiency
decreases with temperature and, characteristically, higher temperatures decrease the total luminescent yield
[Akselrod et al. 1998]. Bular and Göksu [1998] and Sommer et al. [2008] investigated the use of Thermalox R ,
a commercial form of BeO,11 for dosimetry with promising results.
Other Synthetic Materials There are numerous other synthetic materials that have been investigated
for OSL dosimetry. However, none are as promising as Al2 O3 :C and BeO, mainly because of the high
fading from shallow traps exhibited by these other materials. These alternatives include MgO:Tb3+ [Bos
et al. 2006], MgSi2 O4 :Tb, Al2 O3 :Cr,Mg,Fe, MgAl2 O4 (cubic spinal crystals), Brazilian fluorite (CaF2 ), and
various barium aluminoborate glasses (20Al2 O3 ·50B2O3 ·30BaO) [Yoshimura and Yakihara 2006]. Potassium
compounds, such as KBr:Eu, KCl:Eu, KBr:Cu+ , and KBr:Cu+ , have also been investigated as OSL materials
[Nanto et al. 1993; Douguchi et al. 1999; Bandyopadhyay et al. 1999] and they all have relatively short decay
times of about 1 μs. All have a luminescent emission near 420 nm and the optimum stimulation wavelength
for KBr:Eu is 620 nm and for KCl:Eu is 560 nm. Problems associated with these potassium-based materials
include substantial fading and the high effective Z of 18.1 and 31.5 for KCl and KBr, respectively, and thus
they overcompensate for doses from low-energy gamma rays.
Kearfott et al. [2015] studied several known thermoluminescent materials for application in OSL dosime-
try, namely LiF:Mg,Tl, Li2 B4 O7 :Cu, CaSO4 :Tm, and CaF2 :Mn. Of these materials, only CaSO4 :Tm pro-
duced appreciable optically stimulated luminescence; however, its luminescent yield was only 10% of the
yield from commercial Al2 O3 :C OSL dosimeters.
Natural Materials Luminescent spectra from several minerals can be used for dating and dosimetry char-
acterization [Krbetschek et al. 1997]. Both thermoluminescence and optically stimulated luminescence have
been used to characterize these minerals, mainly to obtain information on recombination site energies,

11 Developed
by Brush Wellman, Inc., for the thermal and electrical properties of BeO, Thermalox R is now produced by the
renamed Materion Corporation. However, there is no indication of its use for OSL dosimetry in the Materion literature.
984 Luminescent, Film, and Cryogenic Detectors Chap. 19

possible information on trap energies, and also for use in retrospective dosimetry. Possibly the two most
investigated minerals for OSL dosimetry applications are quartz and feldspar, originally studied by Hunt-
ley et al. [1985]. However, difficulties with using natural minerals for dosimetry arise from compositional
differences, activator differences, and various inclusions which usually contaminate natural crystals. Conse-
quently, luminescent spectra are variable and depend on the origin of the mineral. Further, OSL emissions
are a function of the thermal history of the samples, with samples exposed to high temperature having much
lower luminosity [Bøtter-Jensen and McKeever 1996].
For quartz samples taken from archaeological fired clay, Bluszcz and Bøtter-Jensen [1995] determined
that gamma-ray doses of less than 100 mrad (1 mGy) can be measured. Optical stimulation from long
wavelength light (541 nm or 647 nm) produces a single emission band from quartz near 365 nm [Huntley et
al. 1991]. The luminescent lifetime τ of this 365 nm emission is approximately 35 μs. Although Huntley et al.
[1985] first studied feldspar with 514 nm light stimulation, Hütt et al. [1988] discovered that IR stimulation
produced superior results. The optically stimulated emissions from feldspar are much more complex, with
multiple emissions reported by various researchers [Krbetschek et al. 1997], mainly at 280 nm, between 320
to 340 nm, 400 nm, between 560 to 570 nm, and in some cases a broad emission band between 330 nm and
620 nm, with results depending on the choice of OSL filters [Clarke and Rendel 1997; Huntley et al. 1985;
Krbetscheck and Rieser 1995]. Anomalous fading is another problem with feldspars in which trapped charges
are lost by mechanisms other than thermal quenching.
Luminescent Detector Summary
High heating temperatures can lead to non-ideal behavior for some TLDs. IR radiation from the heat source
can cause interference and alter the measured TL spectrum. Also, because several TLD materials may
suffer irreversible damage to the TLDs at high temperatures, a thermal heating limit is often imposed to
prevent such damage. Consequently, deep traps that require temperatures above this thermal limit cannot
be efficiently depopulated. Further, buildup within these deep traps over time causes sensitization of the
TLD and this buildup can also become a source of background emissions during readout.
There are several advantages of OSL over TL. Commercial OSL dosimeters can also suffer damage if
heated to too high a temperature because of damage to the binding material. However, because the read-out
process does not require a heating step, OSL dosimeters generally are unaffected by this encumbrance. With
sufficient energy of the stimulation photons, many of these deep traps not only can be depopulated, but can
also be used in the dosimetry measurement. This increased density of useful trapping centers improves the
radiation sensitivity of OSL dosimeters.
The luminescence from OSL dosimeters is very faint by comparison to the stimulation light source, hence
filters must be used to reduce background light. POSL can be also be used to reduce or almost eliminate this
background light, provided that the decay time of the luminescent centers is much longer than the optical
pulse and the stimulation light source duty cycle is relatively small. As with a TLD, once the OSLD is read,
the dose information is lost. However, an OSLD does not necessarily need to be completely cleared during
the measurement process. A spot on the OSLD can be read with a focused laser, leaving the remaining
unilluminated regions for later measurements. Also, an OSL dosimeter may be illuminated for a time that
is small compared to the mean decay time of the trap and can, thus, leave a high density of filled dosimetry
traps for a later measurement.

19.2 Photographic Film


Somehow it seems fitting that near the end of the long journey through this book, which began with the
discovery of x rays from exposed photographic plates, the use of photographic film as a radiation detector is
finally described with some respectable amount of detail. Radiation exposure of photosensitive emulsion was
first observed in 1842 by Ludwig Moser who reported that when certain bodies were brought into contact
Sec. 19.2. Photographic Film 985

with a silver iodide plate in darkness, an image would still form. He concluded that some materials must
be “self-luminous”. There is evidence that natural radiation had also been observed from uranium salts by
Claude Félix Abel Niépce de Saint-Victor, in which a uranyl nitrate sample had been brought into close
proximity of a photo sensitive silver bromide paper sheet [Niépce de Saint-Victor 1857, 1859]. The Niépce de
Saint-Victor experiments were reported to the French Academy of Sciences in 1858, and apparently Antoine
Henri Becquerel was aware of the work, primarily through work of his father, Edmond Becquerel, who
mentioned the findings of de Saint-Victor in his book La Lumiére: Ses Causes et Ses Effets. Regardless, A.
Henri Becquerel was apparently the first to explain and understand the significance of the discovery, having
observed images formed from uranium salts on photographic plates in 1896.

19.2.1 Basics of Photographic Film


Photographic film consists of a photosensitive emulsion spread upon a base material. This base is either made
of glass or a cellulose material such as cellulose acetate.12 Photographic emulsions consist of a binder and
a photosensitive compound, usually a distribution of microscopic silver halide crystals suspended in gelatin.
Silver bromide (AgBr) is the photosensitive compound usually used for nuclear emulsions. The process for
producing photographic film has some interesting aspects. A photographic emulsion can be produced by
adding the two reacting solutions
KBr (Aq) + AgNO3 (Aq) → AgBr (s) + KNO3 (Aq)
to a gelatin. The mixture is heated between 50◦ C to 70◦ C to cause Ostwald ripening of the mixture [Becker
1966]. It is also usual to add ammonia (NH3 ) to the solution, which produces various amine complexes
and forms an ammoniacal emulsion. During this ripening process, the size of AgBr crystals, referred to as
grains, increases by growing between 100 to 1000 times in size. Larger grain sizes are usually associated with
faster emulsions. The speed of the film can be increased by adding a small amount of mustard oil to the
solution,13 which forms particles of silver sulfide (Ag2 S) on the AgBr grains. Afterwards, the emulsion is
shredded and washed to remove excess KNO3 . During a reheat process, in which the product is melted, more
gelatin is added to the emulsion along with dyes and stabilizers. The process of “after-ripening” increases the
sensitivity and affects the contrast, fogging, and storage properties of the emulsion. The finished emulsion
is then applied to the base. The thickness of the finished emulsion varies with the intended use and ranges
from 5 microns up to 600 microns. The AgBr content in common photographic emulsions is approximately
30%, but is increased to up to 80% for nuclear emulsions.
The silver halide grains in the emulsion are believed to be in the ionized state, even though they are in
crystalline form. Exposure to ionizing radiation can cause the ejection of an electron from the halide ion and
the electron subsequently is trapped at an impurity location. It is believed that the silver sulfide specks in
the emulsion may be such locations. A positive silver ion can migrate to a trapped electron site and combine
with the electron, becoming neutral silver. A single silver atom is unstable, and eventually decomposes back
to a silver ion unless more silver atoms accumulate together. The neutral silver atom may also acquire an
extra electron, thereby becoming a negative ion. If a second positive silver ion migrates to the negative
silver ion, they can combine to form a two-atom cluster. This process continues as long as there are free
electrons. Stability requires accumulation of at least three to four silver atoms. The sensitized silver grains
that acquired neutral silver clusters produce a latent image in the emulsion, and it is this latent image that
can then be developed to form a darkened image.

12 Nitrocellulose isconsidered a much better base for film emulsions. Is it produced by soaking cotton in nitric acid. Unfortunately,
it is also extremely flammable, almost explosively flammable. For this reason, cellulose acetate, a much slower burning base
formed from soaking cotton in acetic acid, is a preferred choice.
13 This process was discovered when film speeds were observed to increase for gelatin bases made from the collagen of cows that

had eaten mustard plants.


986 Luminescent, Film, and Cryogenic Detectors Chap. 19

The development process consists of several chemical treatments after the latent image is formed. In
the case of nuclear emulsions used for dosimetry, the latent image may be accumulated over an extended
period, weeks for instance. Photographic films are generally sensitive to visible light and must be developed
in total darkness. The photographic film can be slipped into a light-tight development container for easier
handling. Chemical developers are used to change positive silver ions in the emulsion into stable neutral
silver atoms. This conversion is done more efficiently for silver grains already having silver atom clusters.
The developer chemical has reducing agents attached to a benzene ring. Here the act of reducing refers to
lowering the positive charge of an ion, in this case changing positive silver ions to neutral silver atoms.14
The reduction potential of a chemical indicates the relative ability to reduce the photographic film. It is also
usual to blend two or more reduction agents together to increase the activity [Becker 1966], and two popular
reduction agents that are used together are metol and hydroquinone. Because the unexposed silver grains
can also become developed, the developer temperature and development times must be strictly controlled to
avoid over- or under-developing the film.
Most developers have several components, consisting of a reducing agent, an accelerator, a preservative,
a restrainer, and a solvent. Because the reducing agent can be slow, an accelerator usually consisting of
an alkali metal compound is added to the developer. Although KOH and NaOH work well as accelerators,
they can also cause softening of the emulsion [Larmore 1965]. Effective accelerators include Na2 CO3 and
K2 CO3 , but release CO2 gas that can cause film blistering if the development temperature is above 27◦ C.
Less effective, but adequate accelerators that do not soften the gelatin and do not release gases include
Na2 B4 O7 (borax) and NaBO3 (sodium metaborate). Because the developer is designed to chemically reduce
the silver halide, it also has a strong affinity for oxygen, and can become ineffective over time. Preservatives
are added to the developer to mitigate oxidation and prolong the developer lifetime. Sodium sulfite (Na2 SO4 )
is one of the most commonly used preservatives. Although Na2 SO4 reacts with oxygen, it does not adversely
affect the development process, and it also prevents oxidation products (such as negative bromine ions) from
accumulating on the film. These halogen ions decrease the pH of the developer. Further, the excess alkali
metal ions added to accelerate the emulsion development can also fog the film, an effect that appears as a
general darkening of the emulsion. Hence, a restrainer is also added to balance the pH during development,
which, interestingly, turns out to be more bromine ions (often KBr). An overall chemical balance is achieved
by adding excess alkali metal ions to the developer, which is compensated by the excess bromine ions. The
addition of the small number of bromine ions released during development is insufficient to upset the chemical
balance. Finally, a solvent is used to dilute the developer concentrate and, in most cases, is simply water.
To quickly stop the film development, the film is soaked in a stop bath solution, usually an acetic acid
solution, that neutralizes the development process. Although the stop bath step is not strictly necessary,
and thorough rinsing with water can be substituted, the development process continues, even if it is at a
lower rate, unless a stop bath is used. Once the film is developed, the remaining undeveloped AgBr must be
removed and is accomplished by fixing the emulsion. Otherwise, the film continues to darken when exposed
to light. The fixer step is performed by soaking the film in a solution of sodium thiosulfate (Na2 S2 O3 ),
which dissolves the remaining AgBr crystals. The film is then thoroughly washed in water and dried. The
darkness of the image that is formed gives a measure of the ionizing dose absorbed by the film and can be
measured with a densitometer.

19.2.2 Photographic Film Characteristics


There are several important film properties that determine the adequacy of a film to perform well as a nuclear
emulsion. Among these properties are the contrast, film speed, and the linearity of the film with exposure.

14 Contrarily, oxidation is a chemical process that causes an atom or ion to lose an electron to become more positive.
Sec. 19.2. Photographic Film 987

These properties are discussed below through a description of the general characteristics of photographic
film.
The Characteristic Curve
The passage of ionizing radiation through photographic film generally deposits only a small amount of energy
in the emulsion. For visible light, the film may actually absorb all energy of the incident radiation. However,
for x rays, gamma rays, and beta particles, generally only a small portion of the radiation energy is deposited.
The absorbed energy produces a proportional amount of ionization in the emulsion. Hence, film provides a
measure of the total ionization produced in the film over a period of time, and so film should be thought of
as a type of time-integrating radiation detector.
After exposure, the opacity of a film emulsion is mea-
sured to determine the absorbed ionization. The opacity D
C E
is measured by the amount of visible light transmitted

Density
high
through the film. The film density D is the ratio of in- contrast
low
cident and transmitted light, or I0 /It . Traditionally for contrast
most radiation absorption applications, this relationship
is determined by an exponential expression, but this is
B
not so for photographic film. Instead, the density is de- A
termined from the transmitted intensity on a base 10 G J log10(It)
logarithmic scale. Hence, the density of the image on
film is generally expressed as Figure 19.35. The characteristic, or H-D, curves for high,
medium, and low contrast films depicting typical features.
The dashed line indicates a location on the H-D curves all
I0 having the same density for different exposure intensities.
D = log10 . (19.52)
It

The density of unexposed film is 0, while film with a density capable of blocking 90% of light would have a
density of 1. To achieve a density of 2, then 99% of light must be blocked, increasing to 99.9% for a density
of 3, and so on. The response of film to ionizing radiation can be documented with the characteristic curve
that is a plot of the film density versus log10 of the transmitted light intensity as depicted in Fig. 19.35. The
characteristic curve was first reported and employed by Hurter and Driffield [1890] as a film characterization
method.15 The region between A and B in Fig. 19.35 is the toe of the curve, while the region between C and
D is the knee of the curve. The region between B and C is a nearly linear function of density versus log10 (It )
and is the most useful portion of the film characteristic. In the region between D and E, film overexposure
causes the density to actually decrease because a latent image reverses from a negative image to a positive
image, an effect referred to as a solarized image. The consequence for dosimetry is obvious, namely in this
region a higher dose diminishes the density and results in an underestimate of the dose.
Contrast
The contrast of the film, denoted γ, is the slope of the characteristic curve region between points B and C,
i.e.,
D1 − D2
γ= , (19.53)
log10 (It1 ) − log10 (It2 )
where D1 and D2 are any two different densities on the curve. High contrast films have γ > 1 while low
contrast film has γ < 1. The implication is that high contrast film exhibits more sensitivity to small exposure
differences than low contrast film. However, the dynamic range of exposure, referred to as the film latitude,
is greater for low contrast film, that is, it takes more absorbed energy to push the density into the knee

15 Sometimes the curve is referred to as the H-D curve after Hurter and Driffield.
988 Luminescent, Film, and Cryogenic Detectors Chap. 19

(a) (b) (c)


Density

Density

Density
0.1

log10(It) log10(It) log10(It)

Figure 19.36. Ambiguity with early speed designations, showing H-D curves with (a) the same
inertia but different latitudes, (b) the same intersection at D = 0.1, but with different latitudes, and
(c) the same Scheiner speeds, but with different latitudes.

region. Although film has a characteristic latitude for the recommended development process, the contrast
is also a function of developer type and development time. Hence, there is some degree of control over the
film contrast through changes in the development process. Low contrast films often have a wide distribution
of grain sizes with the large grains sensitive to low levels of light while the small grains require a greater
exposure before accumulating enough stable Ag atoms to produce a developable image.
The Speed Index
The amount of absorbed energy that is required to produce an image is largely dependent on the speed of a
film. Unfortunately, there are numerous speed indices for films. Three historically popular speed indices are
depicted in Fig. 19.36. One system referenced the inertia of a film, which in Fig. 19.35 is the distance along
the log10 (It ) axis from point G (the origin) to point J where the linear portion of the characteristic curve, if
projected, would intersect the abscissa. This speed rating presumes that a smaller inertia indicates a larger
γ, but this is not necessarily true.
The Scheinergrade (Sch.) system was introduced by the German astronomer Julius Scheiner in about
1894. The Scheiner number is based on the minimum exposure threshold required to produce a latent image
(point A in Fig. 19.35), but even this system for a speed index can produce ambiguous results, mainly because
this index is based on an unused portion of the characteristic curve. The Scheiner number is reported in
degrees between 1◦ (Sch.) to 20◦ (Sch.). A 19◦ increment √ produced a 100-fold increase in the sensitivity
while a 3◦ increment almost doubles the sensitivity ( 19 100 = 2.06914...  2).
The DIN (Deutsches Institut für Normung) speed index system, which replaced the Schneiner system in
1934, refers to the exposure required to produce an image density of 0.1 on the film. Similar to the Scheiner
number, the DIN number is expressed in degrees, but the increment to 100-fold increase in sensitivity is 20◦
instead of 19◦ . Further, the system is based on a log10 scale so that the exposure increase is
S = 10DIN/10 . (19.54)

A DIN increase of 3 would indicate a doubling in speed (10 = 1.9953...  2). For instance, a film with
3/10

DIN 27 would be double in speed to film of DIN 24. Again, this system does not necessarily produce an
accurate depiction of γ. This system, originally developed for black and white film, was superseded in the
1980s by the ISO system.
Edward Weston and his father founded the Weston Instrument Corporation which made one of the first
photographic light meters. One of their employees, William Goodwin, who designed the light meter also
invented the Weston film speed index which was based on the exposure required to make the image density
equal to γ. This system was introduced in the early 1930s. About the same time, General Electric introduced
its own film speed rating system called the GE film values. However, both the Weston and GE systems were
replaced by the ASA system in the 1960s.
Sec. 19.2. Photographic Film 989

Based on early work by Kodak and inspired by the Weston and GE film speed systems the American
Standards Association16 produced the ASA system in the 1950s. The ASA system follows the rule of
reciprocity in which the amount of energy needed to produce a specific density on the film on the linear
portion of the characteristic curve was inversely proportional to the film speed. Hence, film with rating
400 ASA would be twice as fast as 200 ASA and require half the exposure to produce equal density on the
characteristic curve.
The International Organization for Standardization combined the qualities of the DIN and ASA system
to produce the ISO number for speed, which uses the linear ASA number and the DIN number in degrees,
denoted as ASA/DIN. For instance, a DIN number of 21 is equal to ASA 100 and ISO 100/21◦. This system
with several revisions is the current system used by most film manufacturers.

Example 19.1: Given a film package marked DIN 24, what is the equivalent speed in ASA and ISO?

Solution:
Noting that DIN 24 is 3◦ greater than DIN 21, we know that the film is doubled in speed. Hence

ASA = 10(24−21)/10 × 100 ASA  200 ASA.

Also, the ISO designation would then be 200/24◦ .

Fast films usually have large grain sizes in the emulsion, while slow films have substantially smaller
grain sizes. The advantage to the fast film is that they are useful for low exposure situations, but have the
disadvantage of compromised resolution (graininess). The slower films require more exposure to produce a
latent image, but have much higher image resolution.
Non-Linear Effects
Photographic film fails in low light to record an image whose density is linear with accumulated exposure,
an effect known as reciprocity failure. A classic example of this effect is encountered in astrophotography in
which celestial images take several minutes to hours for proper exposure. If the time between the reduction of
individual Ag+ ions is long compared to the dissociation time of a single Ag atom, then a latent image takes
longer to form than predicted by reciprocity. Further, during the exposure time, the photographic emulsions
are exposed to oxygen and possibly moisture in the air. The gelatin is hygroscopic and can absorb water
moisture, thereby incorporating contaminants in the film emulsion. These contaminants act as oxidizing
agents and compete for the isolated Ag atoms, thus causing them to decompose to Ag+ before stabilizing
with Ag clusters. Consequently, absorbed energy information is lost, and the law of reciprocity fails. In
some cases, reciprocity failure in a photographic emulsion can be so severe that no additional amount of
low-level light exposure increases the density of the latent image. In such situations an equilibrium condition
is established in which the number of Ag+ ions capturing electrons is equal to the number of Ag atoms losing
an electron.17
Because the radiation environment is usually low for most radiation workers, the period between ionizing
interactions is typically long compared to an astrophotograph exposure. However, Becker [1966] and Herz
[1969] note that a single energetic electron interacting in the film most likely produces enough localized

16 Now the American National Standards Institute or ANSI.


17 Complicated processes were developed to reduce reciprocity failure with astronomical emulsions, including reducing the pho-
tographic emulsion temperature with dry ice or LN2, and drying the film in a pure hydrogen environment. The former process
used an instrument named a cold camera and the process was named hypersensitization.
990 Luminescent, Film, and Cryogenic Detectors Chap. 19

excited electrons to effectively produce Ag clusters. Hence, the reciprocity failure effect is less pronounced
for this type of exposure than for exposures produced by low intensity and low energy (optical) photons in
which one photon statistically produces a single silver ion.
As a consequence, low-intensity reciprocity failure is of little concern with most photographic films used
for dosimetry. For high-energy gamma rays, the energy passed to photoelectrons or Compton electrons,
as well as secondary ionization electrons, leads to the asymptotic minimum ionizing power of 380 eV per
micron. Chassende-Baroz [1961] demonstrated that such a low ionization power can cause reciprocity failure
for slow photographic emulsions.
Another form of reciprocity failure is caused by excessive exposure that propels the film density past
the knee region of the characteristic curve, producing a solarized image of reduced density. Ehrlich and
McLaughlin [1956] and Ehrlich [1956] show that the effect can be severe, and is a function of irradiation
rate and dose. At high enough doses, x-ray films were shown to return nearly to zero density, as though
the samples were barely exposed at all. The tested films reached the knee of the H-D curve at exposures
between 10 R up to 200 R, depending on the irradiation rate (R s−1 ).
Another source of dosimetric uncertainty is related to the variation in time of how the film is exposed to
radiation, or the so-called intermittency. For low to medium exposures, the image density of the photographic
film falls in the linear portion of the H-D curve. If the film is exposed to radiation intermittently over time,
the density of the latent image increases additively with total exposure. In fact, it is this property that
makes photographic film an important integrating dosimeter. However, for high total exposures generally
exceeding 10 R, intermittent exposure can cause reciprocity failure and solarizes the film. Results from
Ehrlich [1956] indicate that intermittent exposures can actually cause solarization at lower exposures than
continuous exposures, even though the irradiation rates are identical during the exposure periods.

19.2.3 Film Dosimetry Badges


Personnel dosimetry film badges once were widely used, although TLDs and OSLDs have now replaced film
in many applications. Regardless, photographic film emulsions can be used to measure dose from x rays
and beta particles. If a neutron reactive foil is
placed adjacent to the film, it can also be used
"# for neutron detection. The film is contained in-
side a film holder or film badge which serves as
 
 a light proof, vapor proof envelope that protects
 !
the film from light, chemicals, and water mois-


ture which would otherwise alter the response


or fog the film.
Dosimetry film has two emulsion layers, one

on each side of a backing layer. One layer is a
fast large grain emulsion, while the other is a
much slower small grain emulsion. Hence, the
large grain emulsion is sensitive to low radiation
exposures, while the smaller grain emulsion is

   sensitive to high radiation exposures. Should
   the fast emulsion be overexposed to radiation,
it can be removed and the slower emulsion be
Figure 19.37. Photon energy dependence on image density for bare used to interpret the dose.
and filtered Du Pont 502 film. The compound filter is composed of
0.5 mm Cu, 0.74 g cm−2 Bi, 0.117 g cm−2 Au, 0.114 g cm−2 Ta, Filters can be used to distinguish among dif-
0.148 g cm−2 Er, and 0.148 g cm−2 Gd. Data are extracted and ferent radiations. For instance, a shield can
adopted from Storm and Shlaer [1965]. be used to block beta particles while allowing
Sec. 19.3. Track Detectors 991

gamma rays to interact in the film. Also, filters can be used to flatten the energy response of gamma rays
by attenuating a portion of low energy photons interacting in the film (see Fig. 19.37). With different atten-
uators over one or more films and with knowledge of the film energy response with each attenuator, a crude
energy response to the total photon fluence can be calculated.
Photographic film has the advantage that it can be preserved as a permanent record of dose, with
accurate response down to 100 mrem. However, disadvantages include the added processing with chemical
development, data interpretation (densitometer readings), and the fact that doses less than 20 mrem are
difficult to analyze. Low doses may be susceptible to reciprocity failure, a form of fading. Also, photographic
film can be fogged if left in relatively high heat for too long.
The position of a film badge on the human body is important. Usually the badge should be worn on the
torso, often clipped to a shirt pocket, a belt near the wasteline, or clipped to a lanyard around the neck.
For persons working in a radiation area with their hands, such as a beam port or with laboratory sources,
special rings loaded with photographic film can be used to measure dose to fingers and hands.
19.3 Track Detectors
Track detectors belong to a class of sensors that can provide visual evidence of radiation interactions. For
instance, the cloud chamber that was introduced in Sec. 9.5.8 is a type of gaseous detector that produces
visible ion tracks made by charged particles. In fact, discussion of the cloud chamber could have been
deferred to this chapter, but because it operates with a cooled saturated vapor and often has a voltage
applied to counter gravitation effects, the authors chose to include it in the chapter on ion chambers. There
are numerous other types of track detectors, many described here, all providing visual evidence of the passage
of radiation through the detector.

19.3.1 Nuclear Track Emulsions


For a photographic film to be used as radiation dosime-
ters, it is assumed that the film is uniformly exposed to
a radiation field so as to produce a uniform density over
the developed film. However, it is also possible to detect
the passage of individual radiation particles from the
tracks they make in the emulsion. Nuclear track emul-
sions are a special type of film with a higher density
of nanoparticle silver halide (AgBr) crystal grains. The
silver halide density can be up to 82% by weight with
grain sizes of about 300 nm. To increase the probabil-
ity that incident radiation particles or reaction products
produced by interactions in the emulsion are completely
captured in the film, these emulsions may be up to 600
microns thick. Individual tracks are produced by high Figure 19.38. Photomicrographs with 8 mm apochromat
(x20) and x10 periplanatic eyepiece. (left) Thorium alpha-
LET particles, and the developed tracks are tediously particle stars; (right) similar tracks after uranium intensi-
visually counted through a microscope. Yet, much in- fication. Reproduced from Powell et al., J. Sci. Instrum.,
formation can be extracted from the tracks, including 23, 102–106, (1946). Copyright IOP Publishing. Repro-
trajectory, energy, and LET. Examples of alpha particle duced with permission. All rights reserved.
.
tracks in film are shown in Fig. 19.38 for film that has been permeated with fine thorium and uranium
dust.
Several charged-particle ranges as a function of energy and mass are shown in Fig. 19.39 for a specific
nuclear emulsion (Ilford C2). Except at low energies below 1 MeV, particle ranges are almost propor-
tional to the initial energy of the particle. Note also that 1-MeV particles have ranges of 2 to 15 microns.
992 Luminescent, Film, and Cryogenic Detectors Chap. 19


At higher energies, generally above 20 MeV, emulsions
exceeding 600 microns are needed, a thickness that can
be realized by stacking several film emulsions together

[De Serio et al. 2005]. Such an emulsion stack allows
the entire track of a particle to be followed. Also, be-
cause the intrinsic interaction efficiency can be low for a

single emulsion layer, use of a stack of emulsion layers,
 therefore, increases the detection efficiency.
Each film layer is called a pellicle, and it records the



track of a particle as it traverses the emulsion of the
pellicle. The stack layers are pressed together to form


  a 3-dimensional block of emulsion and may consist of


several hundred pellicles. Because of non-uniformities
 across the emulsion surface, the pellicles must be pressed
 together with a uniform pressure, recommended as 44 lbs
per square inch [Barkas 1963]. At room temperature,
with the relative humidity kept below 60%, the pellicles
should not stick together. Each pellicle is indexed so
that, after the pellicle stack is developed, the track image
sequence can be followed through the different levels.
To develop a stack, the pellicles are separated and all
are developed simultaneously with or without a backing.
  The simultaneous developing ensures that each pellicle
   experiences the same development conditions. If devel-
oped without backing, each pellicle is suspended in a
Figure 19.39. The range-energy curves for protons, frame protected by a wire mesh on each side. Devel-
deuterons, tritons, and alpha-particles in Ilford C2 pho- opment of a pellicle without a backing produces a more
tographic emulsion. Data are extracted and adopted from
Vigeron [1953]. uniform result throughout the emulsion than if a backing
were used, and the developing time is shortened because
development proceeds from both sides of the emulsion. Further, unequal emulsion swelling, a consequence of
attaching pellicles to a glass backing before development, is greatly diminished. Also, the ionization tracks
can be viewed from both sides of a pellicle without backing. However, pellicles without backings seldom
return to their original dimensions after fixing and drying and this can distort the actual length and geometry
of the tracks. Free pellicles must be handled with great care, and it is possible that they adhere to each
other or other surfaces during the processing. Finally, a free developed pellicle usually does not lay flat, and
so may still require adhesion to a stiff backing.
If the emulsion is developed after attachment to a glass plate backing, the film receives mechanical support
and can be developed in special processing racks. However, during the preparation process that requires
washing of the pellicles, water can be trapped and distort the image. Further, unequal shrinkage can alter
the image. An indexing grid printed on the pellicle can be used to correct distortions. Also, it is usual
for the emulsion thickness to shrink after the development and drying process. This shrinkage changes the
measured track length from that in the original emulsion. However, irradiation with x rays or other ionizing
particles, shadow shielded to enter a select location at a 45◦ angle, can be used to determine the thickness
change [Barkas 1963]. The shrinkage factor can be determined from
lD
S= , (19.55)
Ld
where the variables l, L, d and D are defined in Fig. 19.40.
Sec. 19.3. Track Detectors 993

alpha particle
Nuclear track emulsions can be used to source
study nuclear reactions because a reaction in
the emulsion preserves the energy deposition D
apparent particle
track after development
as a function of position. Measurements of particle track before
these tracks can be conducted by visual in- development

spection under a microscope, but automated d emulsion thickness


processes relieve this tedious method. The after processing
track angle into the emulsion is important emulsion thickness
before processing
to correct for the foreshortened projected Sd
length. Emulsions are used to measure the L l

track length of a particle, the angle and cur-


vature of a particle, scattering angles, star
formation, and various other reaction prod- Figure 19.40. Determination of shrinkage for nuclear emulsions. After
uct results. An example of a nuclear reac- Becker [1966].
tion captured on film is shown in Fig. 19.41.
When exposure is conducted in a magnetic field, the curvature of the track yields charge and mass. Star
formation is an indicator of a reaction, with the resulting reaction products emitted in various directions.
The star formation products may be simultaneous, or the result of decay chains. Neutrons can be measured
by way of recoil protons from the water in the emulsion. Also, reactive materials can be incorporated in
the emulsion to enhance specific reactions of interest (10 B, for instance). Photographic track film was used
to discover a number of subatomic particles, including the π + and π − mesons (pions),18 the K + and K −
mesons (kaons), the Σ+ baryon, and the Λ0 baryon.

19.3.2 Track Etch Detectors


In 1958, Young reported on a technique of etching out the damaged tracks left behind by heavy ions penetrat-
ing a solid material. The substrate under investigation was a LiF crystal bombarded by fission fragments.
After etching in a solution of hydrogen fluoride (HF) and water, pits appear where the fission fragments
damaged the crystal. A few years later, Price and Walker [1962] reported on a similar experiment with
mica that was irradiated by recoil ions from spallation reactions, also etched in hydrofluoric acid. Shortly
thereafter, Fleischer and Price [1963] used the method to investigate damage tracks in polymers, which they
noted could be applied to radiation dosimetry. This technique is recognized as an important alternative
detection method for ionizing radiation dose, and is referred to as track etching [Fleischer et al. 1965a].
Fleischer et al. [1972] point out that the technique of particle track counting is simple, the result produces
a straightforward permanent record (a hole), and there is a natural sharp discrimination between particles
that leave tracks and those that do not. Track etch measurements are useful in radiation dosimetry, as
well as other applications, including dating of geological samples and archaeological artifacts, quantitative
chemical analysis for fissionable nuclei or nuclei susceptible to (n, α) reactions, uranium concentrations in
water and other substances, the measurement of diffusion coefficients in metals, the production of uniform
pores in filters, and many other applications as listed elsewhere [Fleischer et al. 1972; Becker 1973; Fleischer
et al. 1975].

Track Formation
Energetic ionizing particles that interact in a substance can produce a dense track of material damage, an
effect that can be observed in organic and inorganic materials. There are at least four models used to describe

18 CecilFrank Powell discovered the pion by photographic means in 1946, and was awarded the Nobel Prize in Physics in 1950
for the development of the photographic method to study nuclear processes and the discovery of the pion.
994 Luminescent, Film, and Cryogenic Detectors Chap. 19

the observed tracks in inorganic solids, namely the ion-


explosion spike model, the atomic displacement model,
the thermal spike model, and the total energy loss model.
The latter three models may contribute some to the
damage formation, but Fleischer et al. [1975] argue that
they are ultimately improbable explanations of the ob-
served results.
In the displacement model track formation is due to
elastic collisions with the material lattice, which causes
a column of displacements along the ion path. This
model predicts that damage paths should appear more
prevalently toward the end of the particle range and that
these paths should appear equally for nearly all mate-
rials. However, the theory fails to explain the observed
Figure 19.41. Mosaic of photo-micrographs of the ‘ex- results for most ion tracks in materials. Fleischer et al.
plosive’ disintegration of the nucleus of a silver atom by a [1975] point out that there are some special cases where
cosmic-ray particle of great energy. The tracks of twenty- ion displacement does participate as an important mech-
five fragments can be distinguished under the microscope,
including those of protons, α-particles, and heavier nuclei. anism for track formation, mainly for heavy low-energy
Many of the tracks ‘dip’ steeply and end in one of the sur- particles and heavy recoil fragments from alpha particle
faces of the emulsion. Reproduced from Powell and Oc- decay.
chialini, Nuclear Physics in Photographs, Oxford, Claren-
The thermal spike model is based on the assumption
don, 1947; by permission of Oxford University Press.
that intense ionization and excitation of electrons along
the ion trajectory causes rapid heating of the material. This heat is initially confined to a small cylindrical
core around the ion path, which is then rapidly dissipated and cooled by conduction to the surrounding
material lattice. It is proposed that the action of rapid heating and cooling produces distortions and disorder
in the material lattice [Seitz 1949; Bullough and Gilman 1966]. However, the model fails to explain observed
results, and Fleischer et al. [1975] discard this model as an explanation of track formation.
The total energy loss model is based on the stopping power equations of Bethe and Bloch (from Chapter
4). This model assumes that the ion tracks form above a critical stopping power S(E) = −dE/dx, which
depends on the radiation particle, its energy, and the target material [Fleischer et al. 1964]. Below this
critical dE/dx, the tracks become distorted and eventually disappear at sufficiently low particle energies.
However, Fleischer et al. [1965] also discard this model in favor of the ion-explosion model, mainly because
the total energy loss model fails to predict observed results.
The ion-explosion spike model maintains that a heavy ion of sufficient energy causes the dense removal of
electrons from host nuclei by Coulombic attraction. Because of the large mass differences, the electrons are
easily removed and ionized, while the heavy ion trajectory remains unchanged along a straight path. The
remaining dense concentration of positive charge left behind causes repulsion along a cylindrical core, thereby
producing lattice distortions usually on the order of several atomic spacings [Fleischer et al. 1965b; Fleischer
et al. 1975; Nordlund et al. 1998]. Ultimately, the end result is the production of a strained lattice with
vacancies and interstitials produced along the ion path. These weakened regions etch in caustic chemicals at
a faster rate than undamaged regions, and consequently produce a residual visible track. There are various
other theories for track formation [Fleischer et al. 1975], but it is the ion-explosion model that remains the
favored explanation. Price and Fleischer [1971] describe a track formation metric J that depends on the
particle’s atomic number Z and its relative speed β = v/c where c is the speed of light in vacuum, namely
 
αZe2 ln (β 2 /(1 − β 2 )) + K − β 2 − δ(β)
J= , (19.56)
β2
Sec. 19.3. Track Detectors 995

#  $ %"  & 
   

   


2
    

)
 
! " 

!
 1!

 %

 0

/
    
   .

-
  
' ' ( ) % * % + + ,   


          
     

Figure 19.42. The relative density of radiation damage as a function of velocity


for various nuclei. Horizontal lines indicate the approximate threshold required
for several materials before a track forms. After Price and Fleischer [1971].

where K and α are constants, Ze is the effective charge of the projectile ion, and δ(β) accounts for relativistic
corrections. For β  0.8, the term β(δ) is zero. The constant K is chosen experimentally with the boundary
condition that the etch rate depends solely on J (within experimental error). Shown in Fig. 19.42 are a set
of curves, developed from Eq. (19.56) with K = 16. Also shown are experimentally established ionization
thresholds for a variety of materials, showing the dependence on ion mass. Price and Fleischer [1971] note
the actual value of K changes with the type of track material with K being higher for organic materials such
as Lexan than for glass and minerals such as flint glass. Just as fission fragments capture ambient electrons
as they slow (see Sec. 4.5.6), the effective charge Ze of a heavy ion changes, decreasing as the ion loses energy
and captures ambient electrons, an effect that is included in Fig. 19.42.
Visible tracks in organic polymers are apparently related to delta-ray electrons in the specific channel
region of the ion trajectory (see Fig. 19.43). The local dose in the ion track channel can exceed several
Mrad, caused mainly by these delta-ray electrons [Becker 1973]. Further, measurements indicate that the
bulk etch rate of plastics can increase with gamma-ray and electron irradiation [Goland and Mateosian
1973]. Hence, the formation of tracks in organic polymers is mainly attributed to a radiochemical damage
mechanism. The etchable tracks are formed by radiolytic scission of polymer chains into short fragments.
The resulting lower molecular weight fragments are far easier to dissolve than the surrounding undamaged
material. Consequently, etched pits appear as these localized regions etch faster than the surrounding
undamaged plastic.

Track Etching
The damage region from a heavy ion is approximated as a cylinder with a diameter of approximately 5 nm (50
Å). The highest damaged region is at the center of the track with the damage becoming less with increasing
996 Luminescent, Film, and Cryogenic Detectors Chap. 19

vG original surface
q vG
cone
undamaged vT q angle vG t vG t
etched surface
vT vT t 2q
» 50 A particle trajectory l
R

undamaged highly
moderately
damaged D
damaged
region advancing tip particle
of etch pit track

Figure 19.43. Ion damage track and etching on a sub- Figure 19.44. Track geometry with constant VT and VG
microscopic scale. After Henke and Benton [1971]. for a vertical incidence. After Price and Fleischer [1971].

radial distance from the track axis to the track edge, beyond which the substrate remains undamaged (see
Fig. 19.43). The substrate in which the tracks occur and which subsequently are made visible by etching is
often referred to as a track etch foil or simply foil.
The etch rate in the track center is denoted as vT while the etch rate of the undamaged substrate is
denoted as vG . Because the damaged region diminishes radially from the track core, the etch rate in the
track region varies between these two extremes from the track axis to the edge of the track. However, for
the sake of simplicity, consider the case in which the etching rate within the track is constant at vT . With
the notation shown in Fig. 19.44, the depth of the substrate etched away, within time t, from the original
substrate surface is vG t while the depth etched along the ion track is vT t. For an ion trajectory normal to
the track substrate, the net depth l of the etched track is

l = vT t − vG t, (19.57)

in which some of the original ion track is etched away during the chemical etching process. The diameter of
the track at the widest point, after etching, is
1/2
vT − vG
D = 2vG t . (19.58)
vT + vG
Note that both Eq. (19.43) and Eq. (19.44) vanish if vT = vG .
The ratio of the two etch rates is
  1/2
2
vT 2 D 2
= +l = csc θ. (19.59)
vG D 2

Note also, by simple trigonometric manipulations [Price and Fleischer 1971]


⎡   1/2 ⎤
2
D ⎣D D ⎦ = D [tan θ + sec θ] ,
vG t = + + l2 (19.60)
2l 2 2 2

and  2 1/2 ⎡   1/2 ⎤


2
D D
⎣ + 1 D ⎦ = D csc θ [tan θ + sec θ] .
vT t = + l2 + l2 (19.61)
2 2l l 2 2
Sec. 19.3. Track Detectors 997

If the etch is allowed to progress for too long, the track broadens and eventually becomes undiscernible from
background pits. This is especially true if the depth vG t becomes greater than the original ion range R.
For track orientations at angles less than 90◦ to the
target surface, the conic section that intersects the sur- original ion track p
surface
face forms an ellipse instead of a circle (Fig. 19.45). The
actual track position becomes displaced from the center,
v t
more so as angle φ decreases. Also, as φ decreases to- etched G
wards the angle θ, the major axis of the ellipse increases surface
towards infinity. With the notation of Fig. 19.45, the f
geometric relations are
2q r
   
1 r r
φ= arctan + arctan , (19.62) a+p
2 a+p p vT t

and
   
1 r r
θ= − arctan + arctan . (19.63)
2 a+p p

Note that the vertical track etch depth becomes less than Figure 19.45. Track geometry with constant VT and VG
the substrate etch depth if for angled incidence at φ. After Henke and Benton [1971]
and Price and Fleischer [1971].
vG > vT sin φ (19.64)

so that a visible etch pit does not form. Hence, no etch pit forms for angles less than the critical angle,
defined by  
vG
φc = arcsin . (19.65)
vT
Thus to be useful as a track etch material, the track etch speed vT should be much greater than the etch
speed of the substrate vG . As vT becomes greater than vG , the etch pit contrast improves while also the
critical angle φc decreases. Goland and Meteosian [1973] showed for organic polymers that the ratio of etch
rates vG /vT decreases as the total sample gamma-ray dose increases, ultimately becoming unity at a high
enough dose. Under such a condition, where vG /vT = 1, no etch pits form; however, the threshold to enhance
bulk etchability is relatively high, quoted to be above 10 Mrad [Attix 1986].
There are a multitude of etch formulas for the various track etch materials, several of which are listed
in Table 19.2. The etch rate can be altered by changing the solvent concentration and also varies signif-
icantly with the foil type. Although the general trend is an increase in etch rate with increasing solvent
concentration, not all foils exhibit this dependence. For instance, the etch rate for cellulose nitrate does
not increase for concentrations above 6N NaOH solutions and remains relatively constant for higher concen-
trations [Blanford et al. 1970]. Other polymers exhibited increasing etch rates with solvent concentration,
but with varying concentration dependences. Not surprisingly, periodic agitation or stirring of the etchant
solution also increases the etch rate [Becker 1973], most likely a benefit from the physical removal of solute
which, otherwise, would obstruct the fresh polymer surface.
Besides the etchant concentration, other environmental factors can have significant influence on the etch
rate and foil sensitivity. For instance, increasing the etchant solution temperature can significantly increase
the etch rate, and the user should be careful to terminate the process well before the tracks disappear.
There are experimental results that showed a dramatic increase in sensitivity, i.e., number and size of pits,
for some organic foils when irradiated in dry oxygen as opposed to irradiation in a vacuum or nitrogen gas
998 Luminescent, Film, and Cryogenic Detectors Chap. 19

Table 19.2. Etching conditions for several track etch materials. From Becker [1973], Fleis-
cher et al. [1975], and associated references.

Detector Etchant Time Temperature


Material (◦ C)
Minerals
lepidolite mica 15% HF 20 sec 50◦
48% HF 3-70 sec 23◦
muscovite mica 20% HF 2h 23◦
20% HF 12 m 52◦
15% HF 20 m 50◦
48% HF 10-40 m 23◦
phlogopite mica 20% HF 5m 23◦
15% HF 1m 50◦
48% HF 1-5 m 23◦
Glasses
Quartz 48% HF 24 h 23◦
Fused Silica 48% HF 1m 23◦
Borate Glass H2 O 1m 23◦
Obsidian 48% HF 30 s 23◦
Phosphate Glass 48% HF 5-20 m 23◦
Soda Lime 48% HF 5s 23◦
5% HF 2m 23◦
Organics
Cellulose Acetate 28% KOH 30 m 60◦
Cellulose Acetate Butyrate 6.25N NaOH 12 m 70◦
Cellulose Nitrate 6.25N NaOH 2-4 h 23◦
Cellulose Propionate 28% KOH 100 m 60◦
Cellulose Triacetate 28% KOH 60 m 60◦
Cormophenol NaOH 1h 40◦
Poly-Allyl-Diglycol Carbonate (CR-39) 7M NaOH† 24 h 70◦
Polycarbonate 6.25N NaOH 20 m 50◦
Polyethylene 10 g K2 Cr2 O7
+35 ml 30% H2 SO4 30 m 85◦
Ionomeric Polyethylene 10 g K2 Cr2 O7
+35 ml 30% H2 SO4 1h 85◦
Polyethylene Terephthalate 6.25N NaOH 10 m 70◦
(PET, Melinex , Cronar )
Polyimide 25%(aq) KMnO4 1.5 h 100◦
Polymethylmethacrylate sat. KMnO4 50 m 85◦
Polyoxymethalene 5% KMnO4 10 h 60◦
Polyphenoxide 25%(aq) KMnO4 4m 100◦
Polystyrene sat. KMnO4 2.5 h 85◦
Polyvinylacetochloride 25%(aq) KMnO4 30 m 100◦
Polyvinylchloride sat. KMnO4 2.5 h 85◦
25%(aq) KMnO4 2h 55◦
Polyvinyl Toluene (sat aq) KMnO4 30 m 100◦
Silicone-Polycarbonate Co-polymer 6.25N NaOH 20 m 50◦
Siloxane-Cellulose Co-polymer 8N NaOH + Benax 3h 85◦
† Recommended by Kodaira et al. [2016].
Sec. 19.3. Track Detectors 999

Table 19.3. Relative sensitivity of various track etch materials. From Fleischer et al. [1975].

Detector Atomic Least Ionizing


Material Composition Observable Ion
Minerals
Hypersthene Mg1.5 Fe0.5 Si2 O6 100 MeV 56 Fe
Diopside CaMg(SiO3 )2 170 MeV 56 Fe
Augite CaMg3 Fe3 Al2 Si4 O19 170 MeV 56 Fe
Oligoclase Na4 CaAl6 Si14 O40 4 MeV 28 Si
Bytownite NaCa4 Al9 Si11 O40 4 MeV 28 Si
Orthoclase KAlSi3 O8 100 MeV 40 Ar
Muscovite Mica KAl3 Si3 O10 (OH)2 100 MeV 40 Ar
Glasses
Flint Glass 18SiO2 :4PbO:1.5Na2 O:K2 O 2-4 MeV 20 Ne
Quartz SiO2 100 MeV 40 Ar
Silica Glass SiO2 16 MeV 40 Ar
Soda Lime Glass 23SiO2 :5Na2 O:5CaO:Al2 O3 20 MeV 20 Ne
Organics
Amber C2 H 3 O 2 Fission Frag.
Bisphenol A-polycarbonate C16 H14 O3 0.3 MeV 4 He
(LexanTM , Makrofol )
Cellulose Nitrate (Daicell ) C6 H 8 O 9 N 2 0.55 MeV 1 H
Poly-Allyl-Diglycol Carbonate (CR-39) C12 H18 O7 13 MeV 1 H†
Polyethylene CH2 Fission Frag.
Ionermeric Polyethylene (Surlyn ) 36 MeV 16 O
Polyimide C11 H4 O4 N2 36 MeV 16 O
Polyoxymethylene (Delrin ) CH2 O 28 MeV 11 B
Polypropylene CH2 1 MeV 4 He
Polymethylmethacralate C5 H 8 O 2 3 MeV 4 He
(PMMA, Plexiglas , Lucite )
Polyvinylacetochloride C6 H9 O2 Cl 42 MeV 32 S

Polyvinylchloride + C2 H3 Cl + C2 H2 Cl2 42 MeV 32 S

Polyvinyledene Chloride
† Lounis et al. [2001].

environment [Becker 1968]. Becker [1968] also found that exposure to water before irradiation increases the
etching speed of the solvent and the number of visible tracks, and is especially pronounced if the track etch
foil is first soaked in a H2 O2 solution before irradiation. Heinzelmann and Haschke [1971] also observed an
increase in sensitivity when the track etch foils are soaked in ethanol/ammonia before the etching process.
Another method shown to increase sensitivity is to expose the track etch foil to specific wavelengths of UV
light in the presence of oxygen before conducting the etching process [Henke et al. 1970]. This improvement
in sensitivity was found to increase with shorter wavelengths of the sensitizing light. The etch rate also
increases in the presence of an electric field [Tommasino 1970; Tommasino et al. 1981; 1982], with methods
and results reported for various track etch foils [Somogyi 1977; Tommasino 1981; Sohrabi 1981]. Other
factors that can affect the etch rate are bake hardening and foil aging, both methods causing a reduction in
size and number of visible etch tracks [Becker 1973]. A probable cause for the reduction in etch pit density
is thermal annealing of track damage, which causes tracks made by low LET radiation to disappear before
those made by high LET radiation [Attix 1986].
1000 Luminescent, Film, and Cryogenic Detectors Chap. 19

Track Etching for Neutron Dosimetry


The high threshold gamma-ray dose required for track formation makes track etch foils impractical for
gamma-ray dosimetry. Further, heavy charged particles have relatively short ranges in air. Combined with
energy attenuation through the dosimeter package, track etch detectors are a poor choice for heavy charged-
particle dosimeters. Although beta particles may penetrate the encapsulate, it takes high doses before
notable changes occur in the track etch foil [Becker 1973]. However, track etch detectors have utility in fast
and thermal neutron detection, mainly through absorption and scatter reactions. The relative insensitivity
to other radiation interactions is a natural discrimination benefit. Neutron-induced track dosimetry is
performed by (a) first using energy conversion radiator foils to produce energetic neutron-reaction ions that
subsequently enter the track etch foil, or (b) producing neutron-reaction ions from elastic scattering in the
track etch foil itself.
There are a few clear advantages of track etch foils for neutron dosimetry. First, as already stated, they
naturally discriminate background radiations. Second, after etching, they provide a relatively permanent
dose record, and are largely unaffected by the environment if kept at room temperature (no fading). The
development process is straightforward and can be automated, including the readout, which can also yield
highly sensitive measurements. Aside from the obvious visual method, many readout methods have been
developed, including automated optical, radiation, and spark transmission methods [Becker 1973; Fleischer
et al. 1975]. For track etch foils coupled to radiator foils, the dose range is adjustable according to the
density of the fissile element. Finally, the sensitivity can be functionally reduced by separating the radiator
foil from the track foil.
Many materials have trace amounts of uranium, which can produce fission fragments from fast or slow
neutrons. Fissions from slow neutrons depend on the presence of 235 U, which has a much higher fission cross
section than does 238 U but has a significantly lower natural abundance. Hence, the track density depends
on the atomic density and the absorption cross sections of the fissionable nuclides [Becker 2003]. It is by
this means that many of the natural minerals are used for geological age and historical dose calculations,
and many useful minerals are listed in Tables 19.2 and 19.3.
Personnel neutron dosimetry can be performed by outfitting users with a track etch badge. The badge
has track etch foils coupled to radiator foils, often consisting of two samples, one with 232 Th for fast neutrons
and the other with 235 U for slow neutrons. Other candidate converter foils include 237 Np, 239 Pu, and 32 S,
all having different cross sections and threshold energies. The 1/v absorbers 10 B and 6 Li can also be used
as converter foils. By combining different foils with separate track etch dosimeters, a crude estimation of
neutron dose as a function of neutron energy can be determined.

Track Etch Materials


Cellulose nitrate was once a favorite for nuclear track etch dosimeters, mainly because it is relatively sensitive
to low LET ions (see Table 19.3). Direct fast neutron interactions in cellulose nitrate produce energetic H,
C, N, and O recoil ions. The recoil protons do not produce etchable tracks (unless the energy is below
550 keV), yet tracks from the other recoil ions can be resolved. Recall from Sec. 18.3 that fast neutrons
transfer only a small fraction of their energy to the recoiling heavy ion, the fraction increasing as the neutron
scattering angle increases. Consequently, the energy of these recoil ions is much smaller than that of the
initial neutron energy and the track lengths the ions travel are relatively small. However, the visible size
of the tracks can be enhanced by electrochemical etch methods (mentioned above). Recall from Sec. 19.2
(footnote 12) that cellulose nitrate (nitrocellulose) is explosively flammable, and has been largely replaced
with cellulose acetate as a track etch material. Listed in Table 19.3 are numerous other track etch materials
that have utility in dosimetry.
Despite the success of many organic foils, one that stands out as a most useful track etch material
for neutron dosimetry is the polymer poly-allyl-diglycol carbonate (C12 H18 O7 or PADC), or by the more
Sec. 19.3. Track Detectors 1001

common name, CR-39.19 It has a relatively low-energy threshold and is capable of forming etch pits from 13
MeV protons [Lounis et al. 2001], a capability significantly better than that of cellulose nitrate and cellulose
acetate. Attix [1986] points out that a direct correlation between radiation dose and the track density
from proton recoils is not actually possible, although superficially it may seem so. The main reason for the
discrepancy, given by Attix [1986], is that protons of high enough energy do not produce etchable tracks
until their energy is reduced below a threshold.20 Consequently, the track does not correctly represent the
total amount of energy dissipated in the foil. There is also a low energy threshold, below which ions are
undetectable. Although the specific ionization may be high, the small residual track is not visible when
etched [Cross 1986]. When etched by electrochemical assistance at 25 kV cm−1 , the practical lower energy
limit is approximately 50 keV for protons in CR-39.

19.3.3 Spark Chambers


A moving charged particle produces a column of electron-ion pairs in a gas medium. In the earlier discussion
on gas filled proportional and Geiger-Müller counters, it was seen that electrons in a high electric field
were accelerated by the field and could produce even more ionization and excited atoms that ended in a
Townsend avalanche. When the excited atoms deexcite, they can give off visible light which can, in turn,
produce further ionization. This light-producing phenomenon can also be used to create a different type of
particle detector. Such an application was first reported by Greinacher [1934] who described the detection
of alpha-particles with a point electrode near a planar surface. Years later, Chang and Rosenblum [1945]
devised a wire spark counter that accomplished the same task, while eliminating many of the problems
associated with Greinacher’s original design [Payne 1949; Eichholz 1952]. Their device had a single wire
stretched parallel to a metal plate. In 1949 Keuffel devised a counter with parallel metal plates (either Mo
or Cu) spaced 2.5 to 3 mm apart. The surface areas for these parallel plate detectors ranged up to 35 cm2
in order to create a large electrically active region.21 These types of devices are conventionally named spark
counters. Although early versions of spark counters operated in air, pure noble gases are preferred with a
mixture of He and Ne frequently being used [Rice-Evans 1974].
Wire grids or plates stacked parallel to each other can be used to record the tracks of high energy
particles over a very large volume. Such a structure is called a spark chamber. One example is shown in
Fig. 19.46. The wire grid design allows charged particles to pass through the gas while encountering far less
solid material than in the parallel plate design. These devices had multiple stacked planes of wires or plates
so as to produce a large detection volume [Henning 1957]. Early reviews of these chambers were published
by Roberts [1961] and Higenbotham [1965]. A neutron sensitive parallel plate spark chamber (no wires)
which used corrugated metal sheets for the plates was reported by Eicholz [1966; 1969].
Suppose that the high electric field is produced between two parallel plates, with a gas between them, and
an ionizing particle can pass relatively perpendicular to the inner surfaces. In a parallel plate configuration,
the electric field is relatively constant for an applied voltage, and liberated electrons can produce avalanches
along the entire particle path. As the avalanche grows, the build-up of space charge shields the inner-most
charge pairs from the externally applied potential, while the outer most electrons and ions are rapidly drifted
towards their respective electrodes. Hence, the outermost electrons gain energy and produce more ionization.
Rice-Evans [1974] notes that a single avalanche must produce at least 108 free electrons as a condition for
an arc to form. As the charges drift in the gap, these avalanches can combine to produce a relatively dense

19 Columbia Resin number 39.


20 Attix [1986] puts this lower energy limit at 4 MeV; however, the work of Lounis et al. [2001] indicates that it can be as high
as 13 MeV in CR-39.
21 Roberts [1961] notes that Keuffel [1949] was the first to report a parallel plate spark counter, but this work was largely

unnoticed. Not until several others published similar works did it become recognized as important.
1002 Luminescent, Film, and Cryogenic Detectors Chap. 19

Figure 19.46. (left) A parallel plate spark chamber. (right) A cosmic ray track in a spark chamber. These spark chambers
were manufactured and demonstrated by the Physics Department at the University of Coimbra, Portugal.

columnar track of electron-ion pairs creating a low resistance track between the plates so that electrons and
ions can move freely between the plates much like a lightning strike. The excited ions produce light upon
returning to their ground state, light which is observed as an arc or spark discharge. These stages in the
development of a spark are illustrated in Fig. 19.47. The voltage across the gap is usually too low to cause
coronal discharge, but high enough to produce an arc if an ionizing particle crosses the gap.
It is notable that the basic spark counter structure is similar to a simple Geiger-Müller counter. However,
the data recording method is different and much faster for the spark counter than the Geiger-Müller counter.
Recall that the rise time and collection time of a GM Counter is relatively slow, usually having resolving
times between tens to hundreds of microseconds. The process that produces a spark, however, is significantly
faster and does not rely on charge collection. In fact, spark counter responses can be on the order of 10 ns
[Roberts 1961].
Spark chambers can be used to image the passage of cosmic rays and highly penetrating ionizing particles
a shown in Fig. 19.46(right). In order to reduce sporadic arcing and possible damage from coronal discharge,
they are typically not operated under constant high voltage. Instead a gate detector triggers a coincidence
circuit that applies additional voltage to the spark chamber stack, high enough to produce avalanching. The
gate detector can be a pair of scintillators over the top and bottom of the device (depicted in Fig. 19.48).
After the spark occurs, the chamber still has mobile ions between the gaps. These ions can be rapidly
removed with a “clearing field” that is a voltage applied across the spark chamber after the spark event.
Usually the clearing field voltage is applied in the opposite direction to the high voltage and lasts no more
than a few milliseconds. Images of the trajectory of the high energy particle as it travels through the detector,
producing sparks between the plates, can be recorded with a photograph. The device, for instance, can be
operated in darkness and a time-extended photograph can record multiple events. Individual events can also
be recorded by acoustic methods, video, and magnetic sampling methods as explained by Rice-Evans [1974].

19.3.4 Bubble Chambers


Another track detector, the bubble chamber, is closely related to cloud chambers (see Sec. 9.5.8), and these
devices were once important instruments for tracking particles. A reduction of pressure or an increase in
temperature of a liquid can drive the liquid into the gaseous state (see Fig. 19.49). However, under some
circumstances, a liquid can be slowly increased in temperature across the liquid/vapor phase boundary
(from point 1 to 3 in Fig. 19.49), and still exist as a liquid in a metastable state. The same is true if the
pressure is reduced (point 2 to 3 in Fig. 19.49), again producing a superheated liquid in a metastable state.
Sec. 19.3. Track Detectors 1003

_
+++
+
+++++ +++
+
++++++-+
-++-+--++ +++++
--- ----- --
---------------- ++++ +
-
-++-++ --++ -+
-- ----- -- ++
-
+++
+
+++++ ---------+++-+------ + ++ +
++++++-+ - +++++++++++ +++
-++-+--++
--- ----- -- -+ + +
++
--- ----- -- +
---------------- -++-+--++
-
++-++
-----------------
--++ -+
-
--- ----- -- +
+++
+
+++++ --------+-+------- + +
++++ - ++++++++++ +++
++-+
-++-+--++
--- ----- --
---------------- successive +++ ++
-++-+--++ -+ + +
--- ----- -- + ++
++ plasma
-
- -+-+--++
---------------- +
-+
----- -------------- + channel spark
+++
+
+++++
avalanches - -- -+++-+-- +
- ++++++++++ ++
++++++-+
-++-+--++
--- ----- --
+
++ ++
---------------- -++-+--++ -+ ++
--- ----- -- +
---------------- + +++
initial -
-
-++-+--++ -+ +
----- ---+--+--------- +
+++ - --+-++++-+-- + ++ +
avalanches ++++
+
+++++
++-+
-++-+--++
--+++++-+++--++++-+ ++++
--- ----- -- + +++
+
--- ----- --
---------------- ---------------- +
-+-+--++ -+
--- ----- --
- -

-----+++--++++-+-+++-+------
-++++-++
-+---+-+
--- ----- --
----------------
-

charged particle
+
Figure 19.47. Formation of a spark channel at four different times.

scintillation
counter
HV

HV
coincidence
circuit

scintillation
counter
charged particle

Figure 19.48. Depiction of basic spark chamber components. After Rice-


Evans [1974].

Once in a metastable superheated state, a disruption can cause instan-


super-
taneous boiling as the liquid converts to vapor. Examples of disruptive solid critical
stimuli include small bubbles in the liquid, contaminants, and ionization Pc 2
liquid critical
produced by radiation interactions. 1
point

Like the cloud chamber, a bubble chamber has an expansion cham- P 3


t
ber whose pressure can be changed by an attached piston. Unlike a triple point
vapor gas
Pressure

cloud chamber containing supersaturated vapor, the bubble chamber is


filled with a liquid brought up to a temperature just below vaporization
(boiling point). If the piston is rapidly withdrawn, the liquid becomes
spontaneously superheated, and charged particles interacting in the liq- Tt Temperature Tc

uid produce ionization events that erupt into small vapor pockets, or
bubbles [Glaser 1952].22 These bubbles continue to grow in size as the Figure 19.49. A P-T phase diagram,
showing the triple and critical points.
piston is further withdrawn. Cameras are used to photograph the bub-
ble tracks, much as is done with the cloud chamber. Incorporating multiple cameras around a transparent
chamber, or a chamber with view ports, can be used to produce a three-dimensional image of the bubble

22 Donald Glasser received the 1960 Nobel Prize in Physics for the invention of the bubble chamber.
1004 Luminescent, Film, and Cryogenic Detectors Chap. 19

Figure 19.50. This image is taken from one of CERN’s bubble


chambers and shows the decay of a positive kaon in flight. The decay
products of this kaon can be seen spiraling in the magnetic field of
the chamber. Photo courtesy of CERN [1973].

tracks in the chamber. A magnetic field can also be applied to the chamber to cause charged particles to
spin about the magnetic field described by F = qv × B (see Fig. 19.50). Hence, the force on the particle
changes with velocity, and the curvature of the bubble paths can be used to determine the particle velocity
and momentum. Liquid hydrogen is probably the most used medium in a bubble chamber. Other liquids
used include liquid deuterium, a mixture of liquid neon and hydrogen, liquid propane, and bromotrifluo-
romethane (CBrF3 ). Laboratory bubble chambers may be only a few liters in size, while bubble chambers
used for high energy physics can be very large. For instance, the Gargamelle bubble chamber was designed
to hold approximately 12 cubic meters of liquid, while the volume of the Big European Bubble Chamber
(BEBC) contains almost 35 cubic meters. While bubble chambers at one time played an important part in
high energy physics, they have been largely replaced by multiwire gas-filled chambers.

19.3.5 Superheated Drop Detectors


Another type of bubble chamber is the superheated drop detector (SDD), shown in Fig. 19.51. First in-
troduced by Apfel [1979], the device consists of a closed vessel backfilled with polymerized gel saturated
with liquid droplets, usually a type of halocarbon with a boiling point well below room temperature. For
instance, an elastic polymer or gelatin may be saturated with liquified R-12 refrigerant (dichlorodifluo-
romethane, CCl2 F2 ) droplets. The saturation process is usually performed under high pressure [Roy et al.
1987].
These superheated droplets are on the order of 25 microns in diameter. At room temperature, the
halocarbon liquid droplets would ordinarily convert to the vapor phase. However, the pressure on the
gelatinous polymer provides sufficient surface force around the droplets to keep them in the liquid state at
a temperature above their ordinary boiling point. By physically separating and suspending the superheated
droplets in the gel, the phase change of a single drop from superheated liquid to vapor does not cause
additional eruptions. Consequently, the other droplets stay in the superheated state.
Neutron interactions in the fluid produce recoil ions, and these ions can track near or through a super-
heated drop. Recoil ions can produce a trail of vapor embryos inside a drop, which are small vapor bubbles
Sec. 19.3. Track Detectors 1005

Figure 19.51. (left) Components of a superheated drop detector. (right) Before and after neutron irradi-
ation of a superheated drop detector. Photo courtesy of Bubble Technology Industries, Inc., [2018].

on the order of 100 nm diameter. Consider a vapor embryo at a specific temperature T and pressure P . The
critical energy required for bubble nucleation is [Roy et al. 1987; Seth et al. 2013]

16πσ 3 (T )
Ec = , (19.66)
3(Pv (T ) − P0 )2

where σ(T ) is the surface tension23 of the droplet at temperature T , Pv (T ) is the vapor pressure of the liquid
at T , and P0 is the pressure of the emulsion suspension (and the droplet fluid). If the radius of the droplet
exceeds a certain critical radius rc , then the droplet expands until it is entirely converted to vapor. If instead
the radius is less than rc , then it shrinks back into the superheated liquid drop. This critical radius is given
by [Seitz 1958; Roy et al. 1987]
2σ(T )
rc = . (19.67)
Pv (T ) − P0
Through this expansion process, particle interactions within the volume, by both charged and neutral parti-
cles, cause the spontaneous state change of liquid to vapor, forming suspended vapor bubbles on the order of
1 mm diameter. These bubbles appear at the particle interaction locations, and the density of bubbles yields
a measure of the particle interaction density, imparted dose, and, in some cases, the particle flux. Cooling or
repressurizing the emulsion in the vial can, in some designs, return the gas bubbles back into small droplets
in the superheated liquid state and so render the device usable for subsequent measurements.
Unlike the bubble chamber, these detectors are portable and do not require moving parts (such as a
piston). Superheated drop detectors are extremely sensitive to epithermal and fast neutrons, but virtually
insensitive to gamma rays. If chlorinated halocarbons are used, superheated drop detectors can also be
sensitive to thermal neutrons through the 35 Cl(n,p)35 S reaction [d’Errico 2001]. Readout of the devices can
be conducted optically or acoustically.
The optical measurement mode consists of counting the bubbles formed in the chamber, either manually
or with an optical scanner. Another measurement method is to incorporate a graduated expansion tube as

23 Here σ should not be confused with the same symbol used throughout this book for a microscopic cross section.
1006 Luminescent, Film, and Cryogenic Detectors Chap. 19

Figure 19.52. Response of a superheated drop detector Figure 19.53. Thermal response dependence for two types
threshold spectrometer set (Bubble Detector Spectrometer of threshold superheated drop detectors. Black data are
or BDS) from Bubble Technology Industries. Data are from for SDD-1000 and white data are for SDD-6000. Here ◦ =
Ing [2001]. 40◦ C, 2 = 35◦ C,  = 30◦ C, and 3 = 25◦ C. Data are from
Apfel and d’Errico [2002].

part of, or extending from, the vial, much like a thermometer [Apfel 1992]. As bubbles are produced, the
emulsion expands and moves along the metered tube, yielding a rapid measure of the number of bubbles or
the neutron dose. Because the bubbles in the vial are measured after irradiation, these SDDs are considered
to be passive counters that accumulate a radiation response over their exposure time.
If the SDDs are used acoustically, the noise produced by an expanding bubble is measured by transducers
arranged around the chamber during radiation exposure. These transducers are connected in coincidence
mode to discriminate out background acoustical noise. An additional acoustical detector can be added to
operate in anticoincidence to discriminate out vibrational noise from electronics and the readout system. In
some cases, the transducers can be connected at opposite ends of the vile, and the arrival time of the sound
wave at each transducer can be used to localize the 1-dimensional position of the erupted bubble to within
approximately 1 mm [Lim and Wang 1995; 1996]. By adding more microphones, including one inside the
vial, a 2-dimensional localization method can produce a spatial resolution as small as 1.21 mm2 [Felizardo
et al. 2009]. SDDs that report counts in real time are considered active counters.
The threshold for reactions is a function of halocarbon type, emulsion pressure, and the operating tem-
perature. As the temperature is increased, the bubble density for a given neutron exposure may change
significantly [d’Errico 2001]. The neutron energy threshold for bubble formation decreases with increasing
temperature [Apfel and d’Errico 2002], and increases with increasing pressure [Rezaeian et al. 2015]. The
cause may be understood with Eq. (19.67) which shows that an increase in temperature causes the vapor
pressure in the embryo bubble to increase and so results in a reduction in rc . For example, d’Errico [2001]
reports that the value of rc decreases from 326 nm at 18◦ C down to 77 nm at 40◦ C for R-114 (ClF2 CCF2 Cl)
refrigerant. Consequently, a larger fraction of embryos erupt as the emulsion temperature increases and rc
decreases. To counter the effect caused by pressure changes in the nucleated embryos, a small amount of
volatile solvent can be added into the vial above the polymerized gel so as to increase the pressure P0 on
the gel as the temperature rises. This addition helps to counteract the increase in Pv (T ) and a reduction
in the threshold for rc [Apfel 1992]. Although not perfect, Apfel [1992] reports that this method decreases
the bubble formation variation from 0.05 ◦ C−1 to 0.01 ◦ C−1 for the temperature range of 15◦ C to 35◦ C. In
another application, d’Errico et al. [1996] added cooling strips to the vial to keep the temperature constant
during the measurement, thereby eliminating variation in neutron sensitivity with temperature.
Sec. 19.4. Cryogenic Detectors 1007

The strong dependence on halocarbon type, pressure, and temperature can be used to produce a type
of threshold neutron spectrometer based on a set of different SDDs [Bonin et al. 1993; Ing 2001]. Such a
spectrometer is very similar in concept to the foil activation and Bonner sphere methods, discussed in Ch. 18,
for determining the energy spectrum of neutrons. The SDD method uses a set of (usually) six different SDDs
with an unfolding algorithm to provide a relatively rough estimate of important aspects of a neutron energy
profile. Data from a set of superheated drop detectors, named a “bubble detector spectrometer” (BDS), are
shown in Fig. 19.52.
A similar active, acoustically operated, form of superheated drop detector was also described by d’Errico
et al. [1995] and called the bubble interactive neutron spectrometer (BINS). The SDD response to neutron
energy is shown in Fig. 19.53 for two different superheated drop detectors.24 The change in neutron energy
required to trigger an event is large, decreasing by an order of magnitude for both detectors for a temperature
increase from 25◦ C to 40◦ C. This version of a neutron spectrometer has two temperature controlled SDDs
that complement each other over the range of neutron energies to be investigated. This range can be adjusted
for each SDD by changing the SDD temperature. Notice that the threshold energy for SDD-1000 at 25◦ C is
the same as that of SDD-6000 at 40◦ C (see Fig. 19.53) and, thus, provides a smooth transition of sensitivity
over a wide range of neutron energies. Spectral unfolding with the BINS detector can theoretically yield
on the order of 10% FWHM energy resolution for monoenergetic fast neutrons between 250 keV to 5 MeV
[d’Errico 2002].
Superheated drop detectors, or bubble detectors, are used for dosimetry measurements, and match well to
the ICRP 60 recommendations [Portal and Dietze 1992]. Commercial dosimeters and threshold spectrometer
sets are available, along with automatic reading systems.25 The bubbles can be counted and subsequently
recompressed into superheated droplets so that the device can be reused for future measurements. There is
a practical limit on the total neutron fluence that can be measured and is reached when the radiation dose
is so large that bubbles become so numerous that they begin to coalesce. If the bubble density becomes too
high, then it becomes difficult to accurately count the number of bubbles in the vial. For a commercial unit,
this limit corresponds to approximately 300 bubbles. Also, after the initial eruption, the bubbles continue
to slowly grow is size. At some point, it is possible that the bubble grows large enough to damage the elastic
emulsion surrounding the bubble by exceeding the elastic limit. Consequently, the vapor bubble cannot be
recompressed into a superheated droplet. Generally, it is best that the SDD be read and recompressed on a
short time schedule. Ing [2001] recommends resetting on a daily basis.

19.4 Cryogenic Detectors


As discussed throughout this book, there are many detector characteristics to be considered in the design of
an “ideal” energy spectrometer system. Factors such as good intrinsic efficiency and short dead times are
important; but probably the paramount factor is the energy resolution. HPGe systems have largely replaced
NaI:Tl systems as energy spectrometers because of the significantly higher resolution of the former. To
obtain high resolution, a detector must have a small excitation energy to produce a signal carrier so that the
statistical noise is reduced. However, thermal excitation of these signal carriers must be reduced to minimize
electronic noise. This latter requirement means the detector can be operated only at low temperatures.
Sometimes liquid nitrogen temperatures are sufficient as, for example, with HPGe detectors. To achieve
even better resolution, several types of detectors have been designed to operate at temperatures of about 0.1
K. Such detectors are termed cryogenic detectors.

24 These two SDDs originally commercialized by Apfel Enterprises, Inc., are no longer available. The superheated halocarbons in
SDD-1000 and SDD-6000 are C-318 and R-114, respectively [d’Errico et al. 1995], and neither of these superheated halocarbons
is sensitive to gamma rays or thermal neutrons.
25 Bubble Technology Industries, Inc., manufactures these detectors and systems.
1008 Luminescent, Film, and Cryogenic Detectors Chap. 19

Cryogenic detectors can be separated into two broad categories: (1) thermal detectors that measure
temperature changes caused by radiation interactions in the detector, and (2) athermal detectors that measure
charge (or some other signal carrier) produced by the radiation [Friedrich 2006]. Examples of each of these
two types of cryogenic detectors are discussed below. A much more comprehensive presentation by experts
in the field is provided by Enss [2005].

19.4.1 Methods of Cooling


There are several methods used to achieve the low temperatures required for the different types of cryogenic
detectors. In some cases, detectors such as HPGe need only be cooled to temperatures near 77K, achievable
with a liquid nitrogen (LN2) bath, a relatively simple and inexpensive technique by contemporary standards.
Yet, a key requirement for many cryogenic detectors is a means to cool the detector to operating temperatures
below 0.1 K. Typically, cooling to such low temperatures is performed in two or more steps. For lower
temperatures near 4 K, liquid He can be used as the cooling bath which is often surrounded by a LN2
jacket. Liquid He is more expensive than LN2, yet laboratory compressors are available that can provide
this liquid. Although many He-based refrigerators are designed for laboratory use, portable precooling
systems have become available. Finally a second cooling step is used to take the detectors from about 4 K
to mK temperatures. Several such cooling techniques are summarized below.
Precooling Pulse-Tube Refrigerators
Over the past 20 years refined versions of the pulsed-tube refrigerator, introduced in 1954 by Gifford and
Longsworth [1964], offer an attractive method for the initial precooling of cryogenic detectors. The pulse-tube
refrigerator is a He closed-cycle, vibrationless, “dry” device with no moving parts. The lack of vibrations
is critical for most cryogenic detectors. The original pulsed-tube device of Gifford and Longsworth cooled
only to 174 K. In 1984 Mukulin added an orifice to provide resistance to the He flow and, thereby reached a
temperature of 105 K. Since then, various design refinements have continued to lower the temperature of the
cold end of the device to about 4 K, just below the boiling point of He (4.2 K). With a two-stage double-inlet
pulse tube cooler, Wang et al. [1997] achieved a temperature of 2.23 K. Then in the early 2000s an even
lower temperature of 1.73 K was achieved by replacing the He gas, which is mostly 4 He, by 3 He. Today
commercial pulse-tube refrigerators are available from several vendors.26 Hence, replacement of traditional
cryogenic liquids by a modern mechanical cryocooler for precooling makes cryogenic detectors truly portable.
3
He Refrigerators
Many cryogenic detectors require temperatures below a few tenths of a degree kelvin, and various refrigerators
have been developed to produce such low temperatures [Lounasmaa 1974]. A 3 He refrigerator operates by
evaporative cooling of 4 He to produce a 1 K reservoir or pot of 3 He. The liquid 3 He is further evaporatively
cooled to reduce the pot temperature to about 0.2 K. Due to the rarity and high cost of 3 He, it is recycled
in a closed loop within the system. Single-stage 3 He refrigerators go down to about 0.3 K and two-stage 3 He
refrigerators can go down to about 0.2 K.
Adiabatic Demagnetization Refrigerators
A relatively compact system, by comparison to a dilution refrigerator, is an adiabatic demagnetization refrig-
erator (ADR). Adiabatic demagnetization is a single cycle method of cooling, unlike a dilution refrigerator
that operates continuously. Adiabatic demagnetization is also the oldest known method of reducing tem-
peratures below 1 K [Lounasmaa 1974] and was originally introduced by Debye [1926] and Giauque [1927].
The magnetocaloric effect operates by first heating a paramagnetic material with magnetism, a process in
which the entropy is lowered in a magnetic field. The heat is removed by a liquid He bath through a contact

26 see starcryo.com, entropy-cryogenics.com, bluefors.com, oxint.com, and leiden-crygenics.com


Sec. 19.4. Cryogenic Detectors 1009

switch. After opening the switch, the magnetic field is slowly lowered, adiabatically, to keep the entropy of
the coolant paramagnet constant, thereby causing the temperature to decrease. The device can produce low
temperatures on the order of 1 mK. Seminal work for development of the ADR was made by Hagmann and
Richards [1994] whose device sustained temperatures of 100 mK for 100 hours. These refrigerators may have
more than one type of paramagnet. Friedrich et al. [2001] describes such a refrigerator with two paramagnet
stages. The first stage is cooled to about 1 K with a gadolinium gallium garnet (Gd3 Ga5 O12 or GGG), and
a second stage is cooled to approximately 0.1 K with a paramagnetic salt Fe(NH4 )(SO4 )·12H2 O or FAA.
The entire system has LN2 and liquid He cooling tanks. ADRs with CPA (chromium potassium alum) can
go down to about 12 mK and those with CMN (cerium magnesium nitrate) can theoretically reach 2 mK.
However, few cryogenic detector researchers use ADRs. The exception is those in NASA who need them
because ADRs work in zero-gravity environments.

Dilution Refrigerators
The 3 He/4 He dilution refrigerator can produce temperatures down to 2 mK. It has no moving parts in
the low temperature region of the refrigerator, relying solely on the phase change of 3 He and 4 He. For
He mixtures containing more that 6% 3 He, a phase separation occurs at 870 mK. The “denser” phase is
composed almost entirely (100%) of 3 He floating atop a “dilute” phase composed approximately of 94% 4 He
and 6% 3 He. Cooling is achieved by forcing the pure 3 He to move across the phase boundary to the lower
dilute phase, much like evaporation in which the denser phase of 3 He is the liquid and the dilute phase is
vapor. This continued action is achieved by circulating the 3 He with a room temperature pump. The 3 He
is recirculated, going through an LN2 precool step, a liquid helium 4 K precool, finally through several heat
exchangers before arriving at the phase separation and mixing chamber, the coldest part of the refrigerator.
The process of moving 3 He through the dilute phase is endothermic, and consequently, heat is removed from
the system. Dilution refrigerators are effective in producing temperatures below 1 K, but are relatively bulky
devices.

19.4.2 Cryogenic Microcalorimeters


There are a few basic configurations of cryogenic detectors, generally described as thermal/equilibrium
detectors and athermal/nonequilibrium detectors [Friedrich 2006]. Thermal/equilibrium cryogenic detectors
can be described as either bolometers or microcalorimeters, with the distinction that a bolometer measures
the amount of radiation incident upon the device (similar to a current mode device) and a calorimeter
measures the energy of individual interactions in the device (similar to a pulse mode spectrometer). The
origin of the bolometer dates to Langley, who in 1880 invented the device to measure small quantities of
infrared radiation [Langley 1880]. Much later, Andrews et al. [1942] introduced a superconducting version of
the bolometer fabricated from tantalum wire operated at its superconducting transition temperature (3.22
K to 3.23 K).
Cryogenic detectors, bolometers and microcalorimeters, measure thermal energy deposited in a low tem-
perature (mK) absorber. The increase in heat in the absorber is converted into a signal and is, thus, a
measure of the energy deposited by incident radiation. Low temperature operation is required to reduce
thermal noise that would otherwise mask the small signal. There are a variety of thermal detectors, some of
which are reviewed in this section.
The simplest cryogenic detector, and possibly the oldest, is a radiation absorber attached to a thermome-
ter. The absorber and thermometer together are weakly attached to a low temperature reservoir bath or
heat sink. These detectors are called, interchangeably, bolometers, calorimeters, thermal detectors, and other
variants. However, there is a distinct difference in the way that bolometers and microcalorimeters operate.
In either case, a cryogenic thermal detector has an absorber attached to a thermally sensitive electronic
1010 Luminescent, Film, and Cryogenic Detectors Chap. 19

component, usually a thermistor.27 Some designs are monolithic so that temperature sensor is the radiation
absorber itself.
Consider the simple cryogenic detector depicted in Fig. 19.54.
The absorber is heated by incident radiation interacting in it at _
+
−1
the rate Pin (t) (J s ). The total heat capacity of the absorber
is denoted by ca (J K−1 ) and the total heat conductance be- I
tween the absorber and heat sink by g (J K−1 s−1 ). A small radiation V
constant current I flows through the thermistor of resistance R
and creates a voltage V across it. The current in the thermistor thermistor R
generates a small thermal power of Po = IV = I 2 /R, which at
equilibrium, causes the absorber/thermistor to have a temper- absorber ca
ature To . Incident radiation interacting in the absorber raises
the absorber/thermistor temperature and, thus, the resistance
weak link g
of the thermistor changes. This change produces a change in the
voltage V that is measured and used to infer the temperature
change of the absorber/thermistor from its equilibrium value as heat sink
well as to record the occurrence of a radiation interactions in the Figure 19.54. A cryogenic detector has a ab-
absorber. sorber with heat capacity ca coupled to a ther-
The behavior of the detector depends on its design. Consider mistor, both weakly attached with conductance
g to a low-temperature heat sink.
a detector at thermal equilibrium with Pin = 0 for t < 0 with
the absorber/thermistor at temperature To . At t = 0 radiation begins to heat the absorber, producing a
change in temperature ΔT (t) = T (t) − To that is measured by the thermistor circuitry. Conservation of
energy requires
ΔT (t) 1
= [Pin (t) − gΔT (t)] . (19.68)
dt ca
The general solution of this first order differential equation with constant coefficients subject to the initial
condition ΔT (0) = 0 is

exp[−t/τF ] t
ΔT (t) = exp[t /τF ]Pin (t ) dt , t > 0, (19.69)
ca 0

where the time constant τF = ca /g.


If a quantum of radiation deposits energy E in the absorber at t = 0+ , i.e., Pin (t) = Eδ(t − 0+ ), the
output temperature pulse is found from Eq. (19.69) as
E
ΔT (t) = exp(−t/τF ). (19.70)
ca
Typically these devices are used for measurement of low energy infrared and x-ray photons which deposit the
photon energy E in the absorber in a single interaction, although other particles can be detected. Thus the
output from the detector is a pulse with an amplitude proportional to the energy deposited in the absorber
by a radiation particle. The decay tail of the pulse can be made small by making τF very small. If the
average time τγ between radiation interactions in the absorber is large so that τF /τγ  1 then the cryogenic
detector produces a train of output pulses whose amplitudes are proportional to the energy deposited by
each incident photon from which the energy spectrum of the incident radiation can be formed. Thus the
device can be used as an energy spectrometer, i.e., a microcalorimeter.

27 A type of resistor in which the resistance is a function of the temperature.


Sec. 19.4. Cryogenic Detectors 1011

However, if τγ  τF , the output pulses pile up upon the tails of earlier pulses and the device behaves
more like a detector operated in current mode. For steady incident illumination with a flux of particles φ
which, on average, deposit an energy E per interaction in the absorber, the incident power Pin = φμVa E,
where μ is the interaction coefficient and Va is the volume of the absorber. If the illumination of the absorber
begins at t = 0, then, from Eq. (19.69)
φμVa E
ΔT (t) = [1 − exp(−t/τF )] . (19.71)
g
Thus, for times greater than a few τF , the output is a signal that is constant and proportional to the incident
flux φ. Thus in this case the cryogenic device is seen to act as a bolometer. In this simple analysis it is
assumed that the time for deposited energy to be manifested as heat is negligible compared to τF or τγ .
Consequently, by changing the readout circuit of a thermal detector, the device can be operated as
either a bolometer or calorimeter. For radiation energy spectroscopy, it is the microcalorimeter that is of
most interest. There are many types of microcalorimeters, yet these devices are separated into two classes,
thermal/equilibrium detectors and athermal/non-equilibrium detectors. Disadvantages of these detectors
include their small volume, which places a practical limit on measurable photon energies, their relatively
slow responses (which limit the measurable gamma-ray interaction rates), and their need for low operating
temperatures. Friedrich [2006] describes these various microcalorimeters in a review article, summarized
here in the following subsections.
Energy Resolution Thermal or equilibrium cryogenic detectors consist of a radiation absorber with heat
capacity ca attached to a thermometer (usually a thermistor). The absorber and thermometer are weakly
coupled to a cold bath by a conductance g. Photon absorption increases the absorber temperature according
to Eq. (19.70) in proportion to the absorbed energy E. The resulting temperature change is measured by
the thermometer before the absorber relaxes to the bath temperature. However, thermal fluctuations of
4gkT 2 limit the energy resolution. These resolution-limiting thermal fluctuations are a result of the random
exchange of phonons across the weak thermal link.
For a fixed absolute T , the total energy of the absorber is ca T and the average energy of the phonons
is kT . The ratio of these terms gives the average number of phonons, N p = ca /k = σ 2 (N p ) if a Gaussian
distribution is assumed. The variance in the phonon energy is σ 2 (E) = σ 2 (kT N p ) = k 2 T 2 ca /k. The energy
resolution limit, measured by the FWHM of the phonon energy distribution, is [Kerson 1987]
√ 
ΔEFWHM = 2ξ 2 ln 2 σ(E) = 2.355ξ kT 2 ca . (19.72)

Here ξ is a dimensionless parameter that depends on the temperature dependence of ca [Moseley et al. 1984]
which otherwise would be unity. However, the lattice heat capacity is a function of the absorber volume
with a T 3 dependence [McClintock et al. 1984], i.e.,
   3
12π 4 N Va k T
ca = J K−1 mol−1 , (19.73)
5 θD
where N is the atom density and Va is the volume of the absorber. Here
: 2 3 ;
θD = 6π v N , (19.74)
k
referred to as the Debye temperature, in which v is the mean thermal atomic speed.
From Eqs. (19.72) and 19.73, it is seen that the energy resolution improves both as the temperature
decreases and as the absorber volume decreases (to make ca smaller). However, a smaller absorber volume
1012 Luminescent, Film, and Cryogenic Detectors Chap. 19

means fewer radiation quanta interact in the absorber so the efficiency of the detector decreases. This
decrease in efficiency then leads to the use of arrays of small absorbers in an effort to offset the decrease in
efficiency of each absorber. The need for high energy resolution means all microcalorimeters must operate
at temperatures as low as possible and with absorbers that are as small as possible, but with sufficient size
to produce an acceptable detection efficiency.
Early microcalorimeters used semiconductor thermistors as the temperature sensor. An x-ray absorption
causes the resistance in the thermistor to increase which produces a change in voltage across the thermistor
for current biased devices. These measured voltage changes can be used to infer the ΔT change in the
detector as a result of a radiation interaction in it. Although effective, as shown by a measured energy
resolution of less than 8 eV for 5.9 keV gamma rays from 55 Fe, the resolution is limited by the heat capacity
of the absorbers.
Microcalorimeters are operated at such low temperatures, near 0.1 K, and with small absorber volumes
that energy resolution of a few eV FWHM is possible only for low energy x rays. The maximum achievable
energy resolution is also a function of Johnson noise in the thermistor, amplifier noise, and photon background
[McCammon 2005a]. Moseley et al. [1984] show that a practical limit is approximately twice the predicted
value of Eq. (19.72). The thermal coupling g between the microcalorimeter is weak at low temperatures,
and consequently these detectors are relatively slow. The thermal pulse decay time τF = ca /g is generally
on the order of 1 ms.
Semiconductor Microcalorimeters
Semiconductor thermistors based on doped Si or Ge are used for high resolution x-ray spectroscopy, and are
probably the oldest type of cryogenic microcalorimeter [Low 1961; Moseley et al. 1984]. These thermistors
require a relatively large change in resistance with temperature (dR/dT ). The absorber can be formed from
a high Z material to improve both the photon absorption efficiency and heat capacity ca ; however, the
material may experience a decrease in thermal conductance between the absorber and the thermistor, ga .
Consequently, the added noise degrades the energy resolution by [Bühler et al. 1994],
  2 1/4
 g g
ΔEFWHM = 2.355ξ 4kT 2ca + . (19.75)
ga ga
As discussed Sec. 12.5.3, the intrinsic charge carrier concentration of a semiconductor increases expo-
nentially with temperature. At low temperatures the number of free charge carriers diminishes to zero,
effectively causing the semiconductor to become an insulator so that it no longer is useful as a thermistor.
The conductivity can be increased by doping the semiconductor with shallow donors or acceptors so the
semiconductor retains some conductivity even at lower temperatures. However, at the very low tempera-
tures required for high resolution microcalorimeters, even shallow dopants enter the “freeze-out” region and
thermal ionization becomes negligible. The work of Anderson [1958] and Mott and Twose [1961] describes
the conduction mechanism of doped semiconductors, including their low temperature behavior. There is a
critical doping concentration below which a semiconductor at 0 K is an insulator but for T > 0 the semi-
conductor retains conductivity [McCammon 2005b]. If the semiconductor is doped slightly below the limit,
the conduction mechanism is governed by phonon-assisted tunneling between impurity sites called “variable
range hopping” (vrh) [Shklovskii and Efros 1984].
For vrh, the electrical resistance can be described by,
p
To
R(T ) = R0 exp , (19.76)
T
where p is approximately 1/2 [Efros and Shklovskii 1975] with R0 and T0 fitting parameters. Equation (19.76)
indicates that ln R(T ) ∝ T −1/2 and is valid over the very low temperature operating range of the detector.
Sec. 19.4. Cryogenic Detectors 1013

Note that Eq. (19.76) indicates that R0 is the resistance at very high temperatures; but Eq. (19.76) is an
approximation valid over only a limited low temperature range and fails at high temperatures. The variation
of resistance with temperature is characterized by the temperature coefficient defined as

d ln R T dR
α= = . (19.77)
d ln T R dT

For R(T ) given by Eq. (19.76)


 p
T0
α = −p . (19.78)
T
The utility of the temperature coefficient is that, for small temperature changes ΔT , the associated change
in resistance ΔR can be estimated from Eq. (19.77) as

R
ΔR = α ΔT. (19.79)
T

The temperature dependence of R for Si and Ge, at first, did not appear to follow the model of Eq. (19.76).
The experimental data varied between samples, at least at the time when measurements were first made.
However, neutron transmutation doped (NTD) semiconductors on Si and Ge [Haller et al. 1996] do, in fact,
follow the prediction of Eq. (19.76) [McCammon 2005b]. This improvement is probably a consequence of the
superior dopant uniformity of NTD along with the reduction of interstitial defects.28 Uniform doping with
deep ion implantation also yields good results [Friedrich 2006].
For high energy resolution, the absorber heat capacity must be kept low, on the order of 10 pJ K−1
[Friedrich 2006]. Bryant and Keesom [1961] found that this requirement for Ge limited the absorber volume
to about 0.001 mm3 . With a typical thermal conductance g of 10 nW K−1 between the absorber and heat
sink, the decay time τF = g/ca is approximately 1 ms [Bühler et al. 1994]. The absorber and thermistor
volumes are kept small to sustain high energy resolution and good performance.
The relatively high specific heat of doped semiconductors, even at low temperature, reduces the sensitivity
of the detector. Kelly et al. [1993] describe a monolithic semiconductor device in which only a small portion
of the semiconductor absorber is doped. Hence, the absorber is the undoped region, and the thermistor is the
smaller doped region, all a part of a single substrate. The composite microcalorimeter has a separate low ca
absorber and thermistor. The combined pair can be optimized to produce a larger device while reducing τF .
To increase the overall volume, these small individual detectors can be fabricated into arrays with individual
absorbers atop each thermistor [Stahle et al. 2004].

Superconducting Transition Edge Microcalorimeters


The electrical resistance of a superconducting material is zero below a transition temperature Tc and exhibits
a characteristic increase in resistance as the temperature is increased above the transition temperature as
shown in Fig. 19.55. The transition temperature changes in a magnetic field, decreasing as the B field is
increased [Rose-Innes and Rhoderick 1978]. Above a critical magnetic field Ho for a Type I superconductor,
superconduction is not possible, even at 0 K. A Type II superconductor has two phases defined by two
limiting B fields. Below TC and the boundary defined by Hc1 , the material superconducts as observed with
a Type I superconductor. However, between magnetic field boundaries defined by Hc1 and Hc2 , the material

28 NTD transforms Ge or Si into dopant atoms through activation, typically n-type dopants, whereas diffusion and implantation
doping replace Ge or Si by forcing them from their lattice locations by the impurities introduced during either the diffusion
drive-in or implantation process.
1014 Luminescent, Film, and Cryogenic Detectors Chap. 19

H (b) H (c)
(a) Hc2
Resistivity

normal
critical normal
Ho magnetic
field mixed state

Hc1
superconducting
superconducting
0 Tc Temp Tc Temp Tc Temp

Figure 19.55. (a) Superconductivity abruptly occurs below a transition temperature


Tc . (b) Type I superconductivity in which the transition temperature Tc is also a function
of the applied magnetic field, with a critical field Ho above which superconductivity is
not possible. (c) Type II superconductor with Hc1 defining the boundary of the mixed
state and Hc2 defining the critical field above which superconductivity is not possible.

transitions into the mixed state, in which both superconductivity and normal conductivity coexist. Conse-
quently, for magnetic fields bounded by Hc1 , Type II superconductors may have two transition temperatures
defined by Tc1 (superconducting) and the other Tc2 (mixed state) above which superconductivity vanishes.29
If a superconductor is set slightly below Tc , then heat added to the system moves the superconductor
above the transition temperature so it no longer has zero resistance. Consequently, current flow through the
material (no longer superconducting) now produces a voltage, which gives a measure of the energy deposited
in the absorber. This type of calorimeter is called a transition edge superconducting (TES) spectrometer.
In normal operation, the device is chilled well below the transition edge, and heated ohmically by applying a
constant voltage bias to the superconducting film that is in contact with the absorber. The bias is adjusted
such that the temperature of the device is maintained slightly below the transition edge. The absorption of
an x ray causes the superconducting film to become normal conducting, thereby increasing the resistance
and decreasing the current.
Because the TES film in contact with the absorber increases in resistance with temperature (just opposite
of that for a doped semiconductor calorimeter), the TES detector can use electrothermal feedback (ETF).
With ETF, the power P = V 2 /R decreases as the resistance increases. Consequently, with lower power, the
return to the cryogenic bath temperature is quicker and the energy resolution is improved [Irwin 1995],
 1/2
4kT 2 C n
ΔEFWHM = 2.355 , (19.80)
α 2

where n is a parameter characterizing the temperature dependence of the thermal conductance as given by
[Irwin 1995]
dP
g= = nKT n−1 . (19.81)
dT
Here K is a material and geometry related parameter. When an interaction event heats the film, the return
to equilibrium is described by
dΔT P0 α
ca =− ΔT − gΔT, (19.82)
dt T

29 Thenormal state is confined to threads of normal cores of conductivity in a triangular pattern with each core surrounded by
superconducting material [McClintock et al. 1984].
Sec. 19.4. Cryogenic Detectors 1015

104
241 241
Am Ge Am
239 238
Pu Pu 241
mCal Pu
Counts / 10 eV bin Pu Ka1
103 Np Ka2 U Ka1
240
Pu
Pu
Ka2

Sn escape
x rays

102 Np Ka1

101
96 98 100 102 104
Energy (keV)

Figure 19.56. Pu spectrum from a microcalorimeter array using data from 11 of 13


active pixels. The combined array resolution is approximately 45 eV. At this resolution,
the broad x-ray peaks can be readily distinguished from gamma-ray peaks. The solid
curve is a spectrum taken with a conventional HPGe detector. c [2009] IEEE. Reprinted,
with permission, from Bacrania et al., IEEE Trans. Nucl. Sci., 56, 2299–2302, [2009].

where P0 is the equilibrium Joule power. When the superconducting film is well below the transition
temperature, P0 = KT n = gT /n, and the pulse time constant is [Irwin et al. 1998],
ca n
τF = . (19.83)
g n + αϕb
Here ϕb is a measure of how far the detector is biased above the bath temperature Tb and is defined as
 n
Tb
ϕb ≡ 1 − , (19.84)
Te
where Te is the equilibrium temperature of the TES calorimeter. Equation (19.83) indicates that high values
of α improve recovery time.
The current is measured through induction with a superconducting quantum interference device (SQUID)
current amplifier. This device is used to reduce amplifier noise because a SQUID does not have voltage noise.
TES calorimeters must have low resistance to ensure rapid and homogeneous thermalization of the absorber
and superconducting film. Typically the choice of absorber depends greatly upon the photon energy of
interest. An energy resolution of 2.37 ± 0.17 eV has been achieved for 5.9-keV gamma rays from Mn Kα
lines using Mo-Au TES thermistors [Iyomoto et al. 2008]. Higher energy gamma rays, yet generally below
100 keV, produce good results with a Sn absorber bonded to superconducting bilayer of Mo and Cu with
a transition temperature of 100 mK [Doriese et al. 2007]. The best reported energy resolution for a single
device was 25 eV for 103-keV gamma rays. Arrays of microcalorimeters can be used to maintain a fast
response time while increasing detection efficiency [Doriese et al. 2007; Iyomoto et al. 2008; Bacrania et al.
2009]. Shown in Fig. 19.56 are comparison x-ray spectra for a typical HPGe semiconductor detector and a
TES microcalorimeter array.
Magnetic Microcalorimeters
Another type of low-temperature microcalorimeter measures the change in magnetism as small amounts
of heat are added to the system. These devices have a radiation absorber coupled to a paramagnetic
1016 Luminescent, Film, and Cryogenic Detectors Chap. 19

sensor, together weakly attached to a low-temperature thermal reservoir [Fleischmann 2005]. Thermal
energy absorbed by the system causes the magnetism to decrease, a decrease which can be measured by an
inductively coupled SQUID.
Originally introduced by W. Seidel in 1986,30 the technology was subsequently investigated for its po-
tential as an ultra-high resolution x-ray spectrometer [Bühler and Umlauf 1988; Bühler et al. 1993; Fausch
et al. 1993; Bühler et al. 1994]. In these original works, energy resolution of 320 eV was achieved for 5-MeV
alpha particles with the compound cerium magnesium nitrate or CMN [see Fleischmann 2005]. However, the
response times were slow with a 40-ms rise times and up to 10-s thermalization times. This slow response,
which is a common problem with paramagnetic dielectric materials, is unsuitable for most x-ray spectroscopy
applications. Bandler et al. [1993] suggested that the response problem can be overcome by embedding mag-
netic ions into a conductive metallic absorber, particularly gold doped with erbium. Fleischmann et al.
[2000] adopted this concept and have extensively studied Au:Er metallic magnetic calorimeters (MMC).
The magnetization change from a paramagnetic sensor is described by [Fleischmann et al. 2005],

∂M ∂M δE
δM = δT = (19.85)
∂T ∂T ca
clearly showing that a small value of ca is required to produce a relatively large change in temperature
and, consequently, a large change in magnetization. The energy resolution of the detector is limited by
[Fleischmann et al. 2003]  1/4
4τ0
ΔEFWHM = 2.355 4kT 2ca . (19.86)
τ1
where τ0 = ca /ga , approximately equal to 1 μs, is the average time for deposited energy in the absorber
to change the spin in the paramagnetic sensor. The time constant τ1 = ca /g describes the time needed for
the (weak) thermal coupling to transfer heat to the low-temperature heat sink. It is notable that MMCs do
not have a bias current, because they are inductively coupled to a SQUID amplifier and thus have no bias
voltage, and therefore do not suffer from resistive heating or associated noise [Enss et al. 2004]. For a fixed
value of ca , MMCs can have better energy resolution than other types of calorimeters, or, instead, have the
same energy resolution but with a larger absorber so that they have improved efficiency. Although these
detectors are relatively slow, they are theoretically capable of less than 1 eV energy resolution. Fleischmann
et al. [2004] reported energy resolution of 3.4 eV for 6.5-keV x rays with a Au:Er MMC, while Gastaldo et
al. [2013] reported 2-eV FWHM for 6-keV x rays.

19.4.3 Athermal Cryogenic Charge Detectors


Another class of cryogenic detectors does not measure thermal effects produced by radiation but instead is
based on measuring the number or the energy of quasiparticles produced by radiation in a superconductor.
Before describing these athermal detectors, some more properties of superconductivity must be understood.
Properties and Mechanism of Superconductivity There is a distinctive difference between a perfect con-
ductor and a superconductor in the presence of a magnetic field. If a perfect conductor is cooled to low
temperatures to obtain zero resistance, and is then introduced into a magnetic field, according to Lenz’s Law
the magnetic field is canceled inside the conductor and effectively dispelled. A similar condition is observed
for superconductors, where the magnetic field is expelled from the superconductor. However, if a perfect
conductor is cooled while already in a magnetic field, the magnetic field continues to permeate the conduc-
tor, and remains trapped in the perfect conductor once the magnetic field is removed, causing the sample to
become magnetized. However, if a superconductor is cooled below the transition temperature in the presence

30 Fleischmann et al. [2005] reference the unpublished thesis of W. Seidel as the introduction of this concept.
Sec. 19.4. Cryogenic Detectors 1017

of a magnetic field, it expels the magnetic field upon being reduced below Tc . This phenomenon associated
with superconductors is called the Meissner effect. Upon removal from the magnetic field, a superconductor
does not trap the magnetic field.
Superconductivity results from the pairing of electrons, called Cooper pairs, created at low temperature
by phonon-electron interactions.31 An electron can cause lattice distortions by attracting nearby positive
atomic nuclei, causing them to move slightly closer to the electron, their movement producing a phonon,
and ultimately appearing as a location with positive charge. This apparent positive charge attracts another
electron, even at relatively long distances on the order of several hundred nanometers,32 and overcomes the
usual repulsion between electrons. These two electrons have opposite spin and momentum and temporarily
form a pair, physically producing a composite boson particle with a lower potential energy than two single
electrons. In fact, the sea of Cooper pairs are represented by a single wave function and follow Bose-Einstein
statistics. They form a state of lowest energy called the condensed state with an energy gap gT between this
condensed state and the lowest energy of two unpaired electrons. This energy gap becomes nearly constant
for temperatures below approximately 0.6Tc.
Cooper pairs do not stay paired, but repair with other electrons, such that the superconductivity condition
is preserved. The energy of the pair is on the order of 10−3 eV, and can be broken by sufficient thermal
energy. Consequently it takes low temperatures to produce substantial numbers of Cooper pairs. If a Cooper
pair is scattered, the total momentum of the pair is conserved and their motion along the electric field lines
is unimpeded. To destroy a Cooper pair, an energy of at least 2gT is required, which is improbable at
temperatures well below Tc . However, the value of gT decreases at the temperature is increased, ultimately
becoming zero at Tc .

Superconducting Tunnel Junction Detector


As just described, gT is the small band gap formed between the Cooper-pair state and the normal state.
The limiting energy gap at 0 K is denoted g0 and is on the order of 1 meV. A semiconductor, such as
silicon, has a band-gap energy on the order of 1 eV, and so the superconducting band gap is 1000 times
smaller. Consequently, the number of electrons changing from bound Cooper pairs into electrons can be
vastly greater per unit absorbed energy. Much like a semiconductor, there is an average energy required to
produce a quasiparticle33 from a broken Cooper pair.
Although the minimum energy must be at least 2gT to make two quasiparticles, the average energy wq
needed to produce a single quasiparticle is slightly more than gT . Initial estimates put the upper limit of
wq at 2gT per quasiparticle [Kurakado and Mazaki 1981a, 1981b]. Later estimates, produced by Monte
Carlo calculations, put the average value of wq closer to 1.7gT [Kurakado 1982]. Consequently, the average
number N  of quasiparticles produced per unit energy in a superconductor is extremely high, an effect which
reduces the statistical fluctuations in the measured signal carriers.34 Ultimately, because approximately 1000
times more quasiparticle
√ charge carriers are produced than in a semiconductor, the energy resolution can be
approximately 1000  32 times better.
Generally the voltage applied to a superconductor causes a current that renders undetectable the small
current changes produced by radiation events. However, the quasiparticles can be measured with a supercon-
ducting tunnel junction (STJ) device. The basic construction of an STJ is a thin layer of insulating material

31 The concept is credited to Leon N. Cooper, who described the idea in 1956. However, it was actually Richard A. Ogg, Jr.,
who first proposed the concept in 1946, ten years earlier than Cooper, but Ogg’s work was apparently disregarded at the time.
32 Yes, this distance is small, but typical lattice spacings are a fraction of a nanometer, so this distance is relatively large by

comparison.
33 A particle whose fundamental behavior is altered by its physical environment. For instance, electrons or holes in semiconductors

are quasiparticles treated classically as particles traveling in vacuum by applying an effective mass.
34 Here N  = E /w .
γ q
1018 Luminescent, Film, and Cryogenic Detectors Chap. 19

sandwiched between two superconducting materials, in which the insulating barrier impedes current flow.
The insulating barrier is made extremely thin such that electrons and holes produced from decoupled Cooper
pairs can tunnel through the barrier. With a potential applied to the device, the tunneling current becomes
a function of the quasiparticle population crossing the barrier [Rando et al. 1992].
To improve detection efficiency and reduce diffusion of quasiparticles away from the barrier, a multilayered
superconducting STJ can be fabricated [Booth 1987; Frank et al. 1998]. The insulating barrier is sandwiched
between two superconductors each with a band gap of gT 1 . On the outside of these superconductors, a much
thicker second superconductor with gT 2 > gT 1 is applied on both sides. The structure forms quantum wells
adjacent to the insulating layer, and thereby assists with confinement of quasiparticles at the barrier. At
least one type of device has Al2 O3 as the barrier (∼ 2 nm thick), Al as the lower gT superconductor
(∼ 50 nm) overcoated with Nb as the higher gT superconductor (∼ 265 nm) [Frank et al. 1998]. Other
STJ detector configurations used Ta instead of Nb [Kraft et al. 1999]. Quasiparticles excited across the
larger energy gap fall into the well by phonon emissions. If a phonon emission is of adequate energy, more
quasiparticles can be excited across the lower energy gap [Mears et al. 1993]. Under a voltage bias, the
quasiparticles tunnel through the barrier and can
insulating
recombine as Cooper pairs on the other side (see barrier
Fig. 19.57).
Booth [1987] describes a quasiparticle multiplier
device that increases the signal by fabricating succes-
sive layers of quantum well tunneling barriers. This
layered structure enables multiple tunneling events to
quantum
occur within some recombination time tr [Mears et al. well
1993]. The effect increases the overall measured signal,
but also broadens the statistical spread in energy reso- e tunneling
gT2
lution. With corrections to the expected energy resolu- egT1
tion including the Fano factor F (≈ 0.2) and statistical
fluctuations in the number of tunneling quasiparticles cooper
(1 + 1/N ), the overall energy resolution is described pairs
backtunneling
cooper
by, energetic pairs
<  
photon
1
ΔEFWHM = 2.355 wq E F + 1 + . (19.87) Figure 19.57. Band diagram of a bilayer superconducting
N  tunnel junction (STJ) detector.

STJ detectors have been reported with energy resolution of 12 eV FWHM at 5.9 keV [Angloher et al. 2001].
Also, for lower energy photons, an energy resolution of 5.8 eV FWHM was measured for 1-keV photons [Kraft
et al. 1999], and 1.9 eV FWHM for 70-eV photons [Friedrich et al. [1999]. The response time is determined
by the time that quasiparticles remain in the quantum well. Their disappearance results from recombination
or diffusion from the region which results in response times of about 3 μs [Friedrich 2006].
Microwave Kinetic Inductance Detectors
In the past ten years a new type of athermal detector has attracted considerable attenuation, particularly in
the astrophysical community, because these detectors can be easily fabricated as large imaging arrays with
high quantum efficiency for photons with wavelengths in the mid infrared (5 μm) to UV photons (0.1 μm).
These detectors are known as Kinetic Inductance Detectors (KIDs) and operate by measuring the change in
kinetic inductance caused by absorption of photons in a thin strip of superconducting material. The change
in the kinetic inductance caused by the liberation of quasiparticles in the semiconductor by the incident
photon is measured as the change in the resonance frequency of a microwave resonator and, hence these
detectors are known better as Microwave Kinetic Inductance Detectors (MKIDs).
Sec. 19.4. Cryogenic Detectors 1019

The seminal paper that began the flurry of interest in these detectors is that by Day et al. [2003], upon
which most of the following discussion is based. Recall that in a superconductor a DC supercurrent, carried
by Cooper pairs, flows without resistance. A Cooper pair, which is bound together by electron-phonon
interactions, has a binding energy wq < 1.7gTc . However, superconductors have a non-zero impedance for
AC currents. An electric field applied near the surface of a superconductor accelerates the Cooper pairs
and, thereby stores energy in the superconductor in the form of kinetic energy. Because the supercurrent
is non-dissipative, the stored energy may be extracted by reversing the electric field. Similarly, energy may
be stored in the magnetic field inside the superconductor, which penetrates only a short distance, λ  50
nm, from the surface. Consequently, a superconductor has a surface inductance Ls = μo λ caused by the
reactive energy flow between the superconductor and the electromagnetic field. The surface impedance
Zs = Rs + jωLs 35 includes a surface resistance Rs to account for AC losses at angular frequency ω caused
by the small fraction of electrons that are not in Cooper pairs, i.e., the quasiparticles. For temperatures
T  Tc we find that Rs  ωLs , thereby having negligible losses in the resonance circuit [Baselmans 2011].
Photons with energy (hν > 2wq ) may dissociate one or more Cooper pairs. The absorption of a high-
energy photon creates Nqp < ηhν/wq quasiparticles where η < 0.57 is the efficiency with which the photon
energy is converted to quasiparticles. The quasiparticles recombine  into Cooper pairs on timescales of
τqp = 10−3 to 10−6 s during which they diffuse over a distance  Dτqp where D is the diffusion constant
for quasiparticles in the superconductor material. Similarly, the absorption of a steady stream of low-energy
(millimeter/submillimeter) photons would raise the steady-state quasiparticle density by an amount δnqp
above its thermal equilibrium value. MKIDs make use of the dependence of the surface impedance Zs on
the quasiparticle density. Although the changes δZs are quite small, very sensitive measurements may be
made using a resonant circuit. Changes in Ls and Rs affect the frequency and width of the resonance,
respectively. These changes, in turn, alter the amplitude and phase of a microwave signal transmitted
through the measurement circuit.
The resonant circuit is often a parallel LC circuit which is capacitively coupled to a coaxial through line.
The effect of the surface inductance Ls is to increase the total inductance L, while the effect of the surface
resistance Rs is to make the inductor slightly lossy (adding a series resistance). On resonance, the LC circuit
loads the through line, producing a dip in its transmission. The quasiparticles produced by the photons
increase both Ls and Rs . These changes move the resonance to lower frequency (due to Ls ), and make the
dip broader and shallower (due to Rs ). Both of these effects contribute to changing the amplitude and phase
of a microwave probe signal transmitted though the circuit.
The choice of a parallel LC circuit coupled to a through line has high transmission at frequencies away from
the resonance and, thus, is very well suited for frequency-domain multiplexing because multiple resonators
operating at slightly different frequencies can all be coupled to the same through line. These detectors can
count individual photons with no false counts and determine the energy and arrival time of each photon with
good quantum efficiency.

Other Athermal Detectors


Superconducting Nanowire Single-Photon Detector A superconducting nanowire single-photon detector
(SNSPD) uses an array of superconducting wires cooled to well below Tc and biased with a DC current just
below the superconducting critical current. Typically these wires are niobium nitride 5 nm thick and 100
nm wide patterned on a substrate. If a photon is absorbed in a wire dissociating Cooper paired electrons, a
small region is created in which the critical current is momentarily reduced below the bias current to form
a small non-superconducting region. A detectable voltage pulse of about 1 ns duration indicates the photon

35 j

= −1 is used to avoid confusion with the multiple uses of i.
1020 Luminescent, Film, and Cryogenic Detectors Chap. 19

absorption event [Natarajan et al. 2012]. Advantages of this detector include its high speed (up to 2 GHz
count rate) and low dark current. However, SNSPDs provide little information about the photon energy.
Roton Detectors The elementary collective excitations in superfluid 4 He are phonons and rotons.36 A
particle interacting in this fluid can produce rotons. These rotons can be detected bolometrically or by the
evaporation of helium atoms [Bandler et al. 1992]. Because 4 He is very pure, rotons travel ballistically and
are stable and thus a large volume of fluid can be used.
Quasiparticles in Superfluid 3 He Below 0.001 K 3 He behaves as a superfluid in which pairs of atoms are
bound as quasiparticles similar to Cooper pairs, ultimately having zero viscosity and flows without kinetic
energy losses. The paired atoms have an exceptionally small energy gap of about 100 neV. Thus a detector
similar to a STJ could be fabricated [Bradley et al. 1995]. The advantage of such a detector is that a huge
number (109 ) of unpaired normal 3 He atoms are produced per particle interaction. But this detector is not
very practical because it is very difficult to detect the normal 3 He atoms and to produce and maintain much
superfluid at such low temperatures.
Capabilities of the Two Classes of Cryogenic Detectors
The principal advantage of charge detectors over microcalorimeters is that the former is much faster [Frank
et al. 1998]. STJs and MKIDs can produce several thousand counts per second per pixel. By contrast,
microcalorimeters are limited to a few tens of counts per second. However, charge detectors, unlike mi-
crocalorimeters, are limited to low energy photons because superconductors cannot sustain electric fields to
sweep out the charges and charges diffuse little before they recombine. Microcalorimeters, while somewhat
more robust in measuring the energy of the radiation quanta, cannot absorb all the energy of very energetic
particles, such as a 10-MeV gamma ray, in their typically small absorbers.

19.5 Wavelength-Dispersive Spectroscopy


Ultra-high resolution can be achieved for low energy gamma and x rays with wavelength dispersive spec-
troscopy (WDS), which can yield x-ray peak resolution better than that of semiconductor or cryogenic
detectors. The method utilizes Bragg scattering, in which the Bragg condition for constructive interference
must be satisfied, i.e,
nλ = 2d sin θ, (19.88)
where n is an integer, d is the spacing between crystalline planes, λ is the wavelength of the photon under
inspection, and θ is the angle at which radiation intersects the crystal from the parallel condition as shown
in Fig. 19.58.
Because it is difficult to make a portable diffraction system, this instrument is generally attached to
an electron microprobe or scanning electron microscope (SEM) [Goldstein et al. 1981]. These instruments
accelerate a focused energetic electron beam onto a sample to produce induced radiations such as secondary
electrons, backscattered electrons (from the beam), and various x-rays as shown in Fig. 19.59. Different
radiation detectors are used with these types of instruments, including gas-filled, scintillation, and semi-
conductor detectors. For instance, secondary electrons are generally detected by a scintillation detector37
shrouded by a Faraday cage, all inside the SEM or microprobe chamber. Backscattered electrons have lower
energy, and because of their wider spatial dispersement, an annular semiconductor detector around the SEM
pole piece is used to detect these electrons. X-ray emissions are often detected with a cryogenically-cooled

36 Rotons are excitations or quasiparticles with a very short wavelength of about 3Å, which is about the same as the spacing
between the helium atoms in the liquid. At temperatures of 1 K and above, it is the rotons which make the main contribution
to the specific heat and the thermal energy.
37 Named a Everhart-Thornley detector after the inventors.
Sec. 19.6. Čerenkov (Cherenkov) Detectors 1021

electron
beam
surface
secondary
l ~ 1 mm electrons

backscattered
electrons

q q characteristic
x rays
d q q
bremsstrahlung

d x-ray
fluorescence

Figure 19.58. Geometry for Bragg diffraction Figure 19.59. Radiations emitted from dif-
of photons. ferent parts of the interaction volume probed
with an electron microprobe.

Si(Li) detector (see Sec. 16.4.1), which yields excellent spectroscopic energy resolution.38 However, in some
cases, higher x-ray energy resolution is required than that provided by a chilled Si(Li) detector and in such
cases WDS can produce the higher energy resolution.
Shown in Fig. 19.60 is a common arrangement for the WDS tool, which allows a sample to be inspected
while it is irradiated with an electron beam which produces characteristic x rays from the sample. These x
rays intersect a slightly bent diffraction crystal. Those x rays satisfying the Bragg condition diffract into a
detector and can be recorded, whereas other x rays are absorbed in the crystal, scatter randomly, or pass
through the crystal. Because only the number of counts at a given diffraction angle need be recorded, the
detector need not be a high-resolution spectrometer, hence a gas-filled proportional counter is usually used
as the x-ray detector. During operation, the crystal and detector are rotated through a Rowland circle,
which permits the Bragg condition to be maintained as the arrangement rotates through a continuum of
wavelengths.
As a result, the x ray detector records the number of counts as a function of wavelength. The stringent
requirement for the Bragg condition results in ultra-high resolution, which can be plotted as a function of
photon energy. The important advantage of WDS is the superior identification ability it provides to the user.
Comparison spectra between a Si(Li) spectrometer, a microcalorimeter, and a WDS spectrometer are shown
in Fig. 19.61. Unfortunately, the system can be used only for photons with sufficiently low energy that Bragg
diffraction can occur. Several commercial systems have a rotating rack of different diffraction crystals that
extend the sensitive range. WDS systems are laboratory-based, hence are not generally considered portable.

19.6 Čerenkov (Cherenkov) Detectors


A charged particle passing through a dielectric material can cause the molecules along its path of travel to
form dipoles, forming a segment of polarization. These molecules promptly return to the relaxed condition by
the spontaneous emission of light, forming wavelets of light to propagate through the dielectric. If the particle
is passing through the material at velocities below that of light in the same media, these successively released
wavelets destructively interfere with each other, resulting in the suppression of luminescence. However, if
the particle is traveling faster than the speed of light in the medium, these wavelets add constructively
to produce a wavefront of light (depicted in Fig. 19.62, left). This pulse of light is known as Čerenkov

38 This method is often called EDS, or energy dispersive spectroscopy, but is the same as energy pulse height analysis.
1022 Luminescent, Film, and Cryogenic Detectors Chap. 19

crystal

crystal q
crystal
q1
electron electron
beam beam q2

l2
detector

l1
sample R detector sample R

2R
Rowland Rowland
circle circle

(a) (b)
Figure 19.60. A typical WDS diffraction arrangement is aligned on a Rowland circle.
The sample location remains stationary. The diffraction crystal is bent with a radius
twice that of the Rowland circle radius R, and it is typically ground with radius R.
The Bragg condition is maintained for various values of λ by moving both the crystal
and detector, with the sample remaining stationary, such that all points remain on the
Rowland circle.
(Cherenkov) radiation, after the Russian physicist who first observed the phenomenon in 1934 by noticing
blue light emissions from water irradiated with gamma rays [Čerenkov 1934; see also Jelley 1955].39
The speed of light c in a dielectric medium is determined by the index of refraction n of the medium as
c
c = , (19.89)
n
where c is the speed of light in a vacuum. If the particle speed v is greater than c , then conditions arise that
produce Čerenkov radiation.40 Consider the diagram of Fig. 19.62(right) in which the distance traveled by a
particle from point A to point C is represented by vt. If the speed of the particle v > c , i.e., v/c ≡ β > 1/n
then the dipoles along its path emit light as the particle slows. The time t for the light wave to travel from
point A to point B is the same as the time needed for the particle to travel from point A to point C, namely
c
vt cos θ = t. (19.90)
n
Rearrangement gives the following condition for Čerenkov radiation emissions
1
cos θ = . (19.91)
βn
There are some important observations to make from this result. First, the particle speed v greatly affects
the light emission angle θ because Čerenkov radiation is emitted anisotropically, i.e., this light is emitted
perpendicularly to the surface of a conical shell subtended by an angle 2θ along the particle path. Second,
if βn falls to unity, then θ goes to zero and there is no emission angle or light emission. As the particle loses

39 Pavel Čerenkov, Il’ja Frank, and Igor Tamm were awarded the 1958 Nobel Prize in Physics for the discovery and interpretation
of this phenomenon.
40 Oliver Heaviside had already predicted Čerenkov radiation in two papers published in 1888 and 1889.
Sec. 19.6. Čerenkov (Cherenkov) Detectors 1023

$V/D
 $O*D$V
0LFURFDORULPHWHU
DE *D/D
('6VSHFWURPHWHU

&RXQWV
$V/E
*D/E
$O.D




EF
:'6VSHFWURPHWHU
  7$3FU\VWDO
&RXQWV






   
(QHUJ\ H9

Figure 19.61. Shown are (top) a comparison of EDS spectra from a Si(Li)
detector and a microcalorimeter detector and (bottom) an additional compari-
son to a WDS detector. Reproduced from Wollman et al., J. Microscopy, 188,
196–223, (1997), with the permission of Wiley Publishing.

of m
ch otio
B er n
en di
ko rec
of m
v r tio
ch otio ad n
er n c iat
en di ion
ko rec
v r tio
ad n
n t
q
iat
ion
A C
vt = bct direction of
particle
direction of
particle
+- +- +- +- +- +- +- +- +- +- +-

Figure 19.62. (left) A particle moving through a medium faster than the velocity of light produces
polar-aligned waves. (right) The angle of light emission is defined by the particle speed and the index
of refraction.

energy through light emissions, the conical angle diminishes and eventually becomes zero. The emission
anisotropy was photographically documented by Čerenkov by irradiating water and benzene with gamma
rays [Čerenkov 1937]. In that experiment, a vial filled with either water or benzene was surrounded by an
angled toroidal mirror to reflect the light up into a camera. The resulting images are shown in Fig. 19.63.
The general outline of the cone is apparent as two fuzzy bright spots in the photographs. Also apparent is
an increase in cone angle with an increase in the index of refraction as predicted by Eq. (19.91).
Frank and Tamm [1937] used Maxwell’s equations to obtain the following expression for the number of
Čerenkov photons emitted, per unit differential path length of travel for a particle with charge number z,
1024 Luminescent, Film, and Cryogenic Detectors Chap. 19

Figure 19.63. Čerenkov radiation from (left) water (n = 1.337) and (right) benzene (n = 1.501). The
semiannular feature is an artifact of the angled toroidal mirror wrapped around the dielectric samples.
However, the two fuzzy bright spots in both photographs do show the perimeter of the emission cone.
Reproduced from Čerenkov, Phys. Rev., 52, 378–379, (1937), with the permission of APS Publishing.

per unit wavelength,


 
d2 N 1 1 2παz 2 : ; 2παz 2
= 2παz 1 − 2 2
2
= 1 − cos2
θ = sin2 θ, (19.92)
dx dλ β n λ2 137λ2 137λ2
where λ is the emission wavelength and α ≡ q 2 /(20 hc) = 1/137.03567 is the mysterious dimensionless
fine-structure constant.41 From Eq. (19.92), it becomes clear that the light yield increases as λ decreases so
that the emission spectrum is greatest in the violet-blue end of the visible spectrum. However, ultraviolet
light is readily absorbed in many dielectrics and, thus, reduces that portion of the spectrum. Consequently,
Čerenkov radiation usually appears blue in color, although many other visible light wavelengths are emitted
but with lower intensities. In the derivation of this expression for Čerenkov radiation, Frank and Tamm
assumed that the index of refraction n is constant, i.e., independent of the light wavelength. However, for
wavelengths in the x- and gamma-ray portion of the spectrum, n decreases to below unity and Čerenkov
emission cannot occur.
The number of Čerenkov photons emitted between λ1 and λ2 < λ1 , per unit path length of travel of the
charged particle, is
 λ1 2
dN d N 2πz 2 1 1
= dλ = − sin2 θ. (19.93)
dx λ2 dx dλ 137 λ2 λ1
Because the most probable wavelengths are also in the sensitive region of most photomultiplier tubes,
Čerenkov radiation can contribute to background for some scintillation detectors, especially organic scintil-
lators. Also, because common glass (n = 1.5) can produce Čerenkov radiation, the glass enclosure of a PMT
can produce background Čerenkov photons and it is especially problematic if the photocathode or first few
dynode stages are illuminated by these photons.
The total threshold particle energy Eth for Čerenkov emission occurs when β = 1/n and is found to be

m 0 c2 n2
Eth =  = m0 c 2
, (19.94)
1 − β2 n −1
2

41 Noone knows why 1/α = 137.03567 or how to calculate it. But if it were to change even slightly, our universe would be very
different. For example, if it changed by even 0.4% fusion in stars could not produce carbon and carbon-based life would not
be possible.
Sec. 19.6. Čerenkov (Cherenkov) Detectors 1025

which includes rest mass energy equivalent m0 c2 . The kinetic energy Tth required to first produce Čerenkov
radiation is found by subtracting the rest mass energy of the particle from the above total energy to give
 
n 2
Tth = m0 c2 −1 . (19.95)
n2 − 1

Compton scattering is the most probable interaction for gamma rays in low Z dielectrics, and the gamma-
ray energy Eγ to produce a maximum energy Tmax of the recoil electron can be found from Eq. (4.74) with
θs = π as 
Tmax + Tmax 2 + 2Tmax mo c2
Eγ = . (19.96)
2
Substituting Tth of Eq. (19.95) for Tmax into
 Eq. (19.96) then gives an expression for the min-
imum energy of gamma rays to produce recoil
electrons that in turn produce Čerenkov radia-

 ! "#$%

tion in a medium with an index of refraction n.


The threshold energies for electrons and gamma
 rays are plotted in Fig. 19.64.
"&&#
Čerenkov detectors are used for a number
 of different applications for the detection of
highly energetic particles, which include gamma
rays (producing energetic electrons), electrons,
    β particles, π mesons, neutrinos, and cosmic
rays. They usually consist of a transparent in-
 teraction medium, such as water or heavy water
          
(D2 O), plastic, or other organic material. At-
  
tached to the absorbing medium are light de-
Figure 19.64. Čerenkov threshold energies for electrons and
tectors, usually photomultiplier tubes (PMTs).
gamma rays as a function of the refractive index. Note that Materials chosen for Čerenkov detectors should
gamma rays can impart only a fraction of energy through Comp- not produce scintillation luminescence or phos-
ton scattering, and therefore have higher Čerenkov thresholds phorescence. For high n materials, the energy
than electrons of the same energy.
threshold is lower and the Čerenkov cone angle
is broader for a given energy. Further, the material should be optically transparent to the Čerenkov emis-
sions. It is also preferred that the absorbing medium be composed of low Z lightweight materials to reduce
scattering and extend the path length of the energetic ionizing particles. A short list of materials investigated
for Čerenkov radiation detectors includes purified water, heavy water, lucite, silica aerogel, benzene, glass,
and various gases (some listed in Table 19.4).
Čerenkov radiation detectors have a fast time response, typically measured in picoseconds. Although
the fast response may have discrimination advantages from other forms of luminescence, this fast timing
property ultimately is limited by the PMT response. The Čerenkov light flashes are relatively dim compared
to those from scintillators consisting of several hundred visible light photons per centimete of particle travel
in the medium. Distinguishing this dim light from background light can be a problem.
The light wave direction and cone angle can be used to determine both particle energy and speed. The
light ring formed by the cone can be projected upon a surface, a method used in Ring Imaging Čerenkov
Counters (RICH) [Seguinot and Ypsilantis 1994; Ypsilantis and Seguinot 1994]. A RICH counter has an
interaction medium adjacent to a reflecting mirror that projects Čerenkov light rings upon a light imaging
sensor. These measurements can also be conducted by arranging multiple PMTs around (or in) the absorber
1026 Luminescent, Film, and Cryogenic Detectors Chap. 19

Table 19.4. Čerenkov detector properties for pure materials.

Refractive Threshold Energy Threshold Energy


Material Index (n) (MeV) (MeV)
λ = 589.29 nm (electrons) (gamma rays)
Air (STP) 1.000277 21.2 21.46
Air (0◦ C) 1.000293 20.6 20.86
Ar (0◦ C) 1.00028 21.09 21.34
H2 (0◦ C) 1.000132 30.94 31.2
He (0◦ C) 1.000036 59.71 59.97
Silica Aerogel 1.0026–1.26 6.589–0.329 6.835–0.498
Liquid He 1.25 0.34 0.511
Water 1.33 0.264 0.423
Water (Ice) 1.31 0.28 0.442
Heavy Water (D2 O) 1.328 0.266 0.425
Water + 10% Glucose Sol. 1.3477 0.251 0.408
Water + 20% Glucose Sol. 1.3635 0.241 0.396
Water + 60% Glucose Sol. 1.4394 0.199 0.3465
Ethanol 1.361 0.242 0.398
Benzene 1.501 0.174 0.315
PMMA (Lucite) 1.49 0.178 0.320
Pyrex 1.47 0.186 0.330
Quartz 1.5 0.175 0.316
Flint Glass 1.6 0.144 0.276
Diamond 2.417 0.050 0.141

and tracking the PMTs that respond to the Čerenkov cone. The Sudbury Neutrino Observatory (powered off
on Nov. 28, 2006) had a 6-m diameter spherical acrylic tank filled with 1102 tons of heavy water, surrounded
by 9600 PMTs. The Super-Kamiokande Neutrino Detection Experiment, or Super-K, has 50,000 tons of
purified water with over 11,100 PMTs surrounding the tank.42
There is an enormous Čerenkov detector array in Antarctica underneath the Amundsen-Scott Pole Sta-
tion, formerly the Antarctic Muon and Neutrino Detector Array (AMANDA), but now officially a part of
the IceCube Neutrino Observatory array. It consists of digital optical modules (DOMs), each containing
one photomultiplier tube (PMT), sunk in the Antarctic ice cap at depths between 1500 to 1900 meters.
AMANDA was originally composed of 677 optical modules mounted on 19 separate strings spread out in a
circle roughly 200 meters in diameter. The newer IceCube array has 60 DOMs per string, with 86 strings
deployed ranging in depths from 1450 m to 2450 m. There are 5160 DOMs in operation within the IceCube
Neutrino Observatory. Each string was placed in the ice by first drilling holes with a hot water hose, lower-
ing the cable string and attached optical modules into the hole, and then the water was allowed to refreeze
around the string.
AMANDA detects neutrinos that pass through the Earth from the northern hemisphere and then react
just as they are leaving upwards through the Antarctic ice. A neutrino collides with nuclei of oxygen or
hydrogen atoms contained in the surrounding water ice, producing a muon and a hadronic shower. The
optical modules detect the Čerenkov radiation produced by these particles, and by analysis of the timing
and location of when and where photons strike the PMTs, the direction of the original neutrino can be
determined with a spatial resolution of approximately 2 degrees.

42 OnNovember 12, 2001, the Super-Kamiokande suffered a severe setback when one of the PMTs imploded and caused a shock
wave in the water that subsequently led to a chain reaction and implosion of over 7000 of the PMTs. The accident occurred
when the water tank was being refilled after routine maintenance. The detector has been rebuilt and is back in operation.
Problems 1027

The IceTop detector array, which is a surface array above IceCube arranged to detect neutrino air
showers, is composed of an additional 320 optical sensors. The main goal of the IceCube experiment is to
detect neutrinos in the energy range from 1011 eV to about 1021 eV.
An additional array called the Deep Core Low-Energy Extension, part of the IceCube Neutrino Observa-
tory, is located in the overall IceCube array at depths between 1760 m and 2450 m. The array location was
chosen for the clarity of the ice at those depths. The Deep Core array is targeted at measuring neutrinos
with energy below 100 GeV and is focused on identifying and characterizing extra-solar sources of neutrinos.
Compared to other large underground neutrino detectors consisting of large water tanks and hundreds of
PMTs, the IceCube is capable of looking at higher energy neutrinos because it is not limited in volume.
However, accuracy is compromised because the PMTs are spaced further apart and the conditions of the
Antarctic ice are not controllable. Traditional neutrino observatories, such as the former Sudbury Neutrino
Observatory or the Super-Kamiokande Neutrino Observatory, were designed to provide greater detail about
neutrinos emanating from the Sun or generated in the Earth’s atmosphere. However, higher neutrino energies
in the spectrum should be dominated by neutrinos from sources external to our solar system.

PROBLEMS
1. Prove the result of Eq. (19.8) from Eq. (19.7).

2. Derive the result of Eq. (19.15) beginning from Eq. (19.13).


3. Both scintillators and TLDs emit photons from radiation absorption, and the phenomenon is used to
measure radiation. Explain the basic difference between these two types of detectors. Why are electron
traps preferred in TLDs but not in scintillators?

4. Consider an extension to the simple model of single-trap level TLD discussed in Sec. 19.1.1. Assume
the traps have a continuous distribution of energies Nte (Et ). Derive an expression for the glow curve
from such a TLD analogous to that of Eq. (19.10) for multiple discrete trap levels.

5. An OSL has decay constant τ = 6 ms and υ = 1 s−1 . Given a duty cycle of 10%, determine the fraction
of measured light from an OSL measurement if (a) τ = 30 ms and (b) if τ = 3 ms. Assume Pr∗ (0) = 0.

6. Discuss the many advantages and disadvantages of a TLD versus an OSLD.


7. Why is the logarithm of the transmitted intensity through photographic film used instead of simply the
intensity to characterize the response of film to light?

8. What is the critical angle for a track etch film where vT = 2vG ?
9. Quartz is perpendicularly irradiated with 5.5 MeV alpha particles with average range of 25 microns.
The track is then etched in a dilute solution of hydrofluoric acid. Given an etch rate of 50 nanometers
per minute for a general undamaged rate, with the damaged rate being 3 times the undamaged rate,
what is the diameter of the track etch after 30 minutes? What is the track length?
10. Derive Eq. (19.78) from Eq. (19.76).

11. Consider the simplified cryogenic calorimeter discussed in Sec.%19.4.2. Calculate and plot the output
N
response produced by a series of impulse inputs, i.e., Pin (t) = i=1 Eδ(t − ti ) where ti = (i − 1)τF /2.
12. What is the minimum electron energy required to produce Čerenkov radiation in flint glass? Compare
this energy to the minimum required energy to produce Čerenkov radiation in pure water.
1028 Luminescent, Film, and Cryogenic Detectors Chap. 19

13. Based on Eq. (19.92), show that the number of Čerenkov photons emitted per unit path length of
charged-particle travel and per unit frequency is independent of frequency and is given by
 
d2 N 1
= 2παz 2 1 − 2 2 .
dx dν β n

Show that integration of this result from frequency ν1 to ν2 > ν1 (corresponding to wavelengths λ1 and
λ2 ) to obtain the number of photons emitted between these two frequencies is the same as that given
by Eq. (19.93).

14. Equation (19.92) suggests that as λ → ∞ an infinite number of Čerenkov photons which have an infinite
amount of energy are emitted. Clearly this cannot be the case. What is the explanation for this false
inference?

15. Derive Eq. (19.96) from Eq. (4.74).

16. Gamma rays of various energies irradiate a translucent material and Čerenkov radiation is observed
when the gamma rays have an energy greater than 1.6 MeV. What is the index of refraction for the
material?

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Chapter 20

Radiation Measurements and


Spectroscopy
Experimental confirmation of a prediction is merely a measurement.
An experiment disproving a prediction is a discovery.
Enrico Fermi

In this book many detectors have been described that respond not only to the presence of radiation but also
have a response that depends upon the energy of the radiation. Unfortunately, the energy response of such
spectrometers is generally not directly proportional to the energy of the incident radiation. Consequently,
the output from such detectors must first be analyzed or unfolded to obtain information about the true
nature of the radiation energy emitted by a source.
By far the most frequently used energy spectrometers are those used to obtain information about x-ray
and gamma-ray sources. In this chapter, methods of analyzing gamma-ray spectra obtained from detectors
capable of energy discrimination are discussed. However, the methods used for gamma-ray spectroscopy
are somewhat general and can also be applied to spectroscopy of other types of radiation. Thus, also
included in this chapter are some basic aspects of charged-particle spectroscopy. Not included here are
energy spectroscopic methods for neutrons, a topic discussed earlier in Chapter 18 on neutron detectors.
The general objective of spectroscopy is to obtain, at a minimum, the qualitative identification of the
source (e.g., source energies or the radionuclides present). However, most spectroscopy applications also
seek quantitative information such as the strengths of the sources or the concentrations of the radionuclides
in a source. Several different methods for qualitative and quantitative analyses are summarized here and
illustrative examples are provided.

20.1 Introduction
Gamma rays and x rays are photons of electromagnetic radiation that are capable of producing ionization
through their interactions with ambient atoms. Technically, x rays differ from gamma rays in their source of
origin but, for practical purposes, this nuance is irrelevant and photon spectra can be analyzed by the same
methods for both x rays or gamma rays. As a practical matter, photons of energy less than about 10 keV
are difficult to detect because they are easily absorbed by the detector housing or source material itself. The
concepts that are discussed here can be applied, in principle, to spectra from photons of energy less than
10 keV and also to spectra generated by other particles, such as electrons. For instance x-ray photoelectron
spectroscopy (XPS) and electron scattering for chemical analysis (ESCA) lead to electron spectra that can
be analyzed by the methods discussed here for photons. Thus, it is understood that reference to gamma-ray
spectroscopy is an oversimplification and many of the methods discussed here can be applied to spectra
generated by x rays, gamma rays, or other types of radiation.

1035
1036 Radiation Measurements and Spectroscopy Chap. 20

Gamma-ray spectroscopy is a general area of study within which spectra are analyzed in order to de-
termine qualitative and, if possible, quantitative information about a sample under investigation. Spectra
generally refer to collections of data for which the independent variable is the channel number (or a related
quantity such as momentum, energy, or wavelength) and the dependent variable is a detector response that
depends on the independent variable. Spectra are generated in many radiation measurement techniques,
such as energy-dispersive x-ray fluorescence (EDXRF), neutron activation analysis (NAA), prompt-capture
gamma-ray neutron activation analysis (PGNAA), electron photoelectron spectroscopy (XPS), and general
counting of unknown radioactive sources. Often, spectroscopy is directed at the quantitative objective of
identifying concentrations of specific elements or isotopes (henceforth the generic term “nuclides” is used)
that are present in samples, but it also can be employed in a qualitative manner to identify whether specific
gamma-emitting nuclides, such as those in special nuclear materials, are present in samples.
In general, a sample to be analyzed emits photons whose energies are characteristic of the nuclides
present in the sample. The emitted photons may arise from excitation from an external energy source or the
sample may emit these photons naturally. A careful spectroscopic investigation generally seeks to determine
either the energies emitted and their intensities or the nuclides present and their concentrations. In previous
chapters on radiation detectors, mainly Chapters 13, 14, and 16–18, examples of radiation measurements with
specific detector materials and configurations have been presented, and the reader is directed to those chapters
for particular detector applications applied to radiation measurements and spectroscopy. For example, the
performance of HPGe detectors is described in Sec. 16.4.2. However, there are measurement and spectroscopy
methods that can be generally applied to most spectrometers. In this chapter, attention is given to photon
spectra that are generated from samples interrogated by any of a number of means, active or passive, to
determine information about the constituents of the sample.

20.2 Basic Concepts


Various photon detectors can provide responses that are proportional to the energy deposited in the detector.
These include proportional counters, scintillation detectors, and semiconductor detectors. Regardless of the
detector, a voltage pulse is created whose amplitude h, generally called the pulse height, is a function of the
energy deposited Ed in the detector, i.e.,
h = f (Ed ), (20.1)
where f is some function. For many detectors, f is linear and

h = α + βEd , (20.2)

where α and β are constants unique to a detector. However, scintillation detectors, in particular, can exhibit
non-linearities, especially at low photon energies (see Sec. 13.2.2), and this non-linearity should be taken
into account. (Linearity of a detector is often expressed in terms of the pulse height per unit energy as a
function of the deposition energy, a quantity which is constant for a linear detector.) In any event, a good
spectroscopist should know f , the functional relationship between pulse height and deposited energy, for any
spectroscopic detector used.
In gamma-spectroscopy, the pulse height h is measured and the deposited energy Ed is obtained by
inversion of Eq. (20.1), namely
Ed = f −1 (h), (20.3)
or, if the spectrometer is linear, then
h−α
Ed = . (20.4)
β
Sec. 20.2. Basic Concepts 1037

Moreover, the pulse heights produced by repeated deposition of energy Ed


in a detector are not exactly the same; rather, they are distributed about
a mean value h0 = f (Ed ) by some kernel g(h|Ed ) such that g(h|Ed )dh is
the probability an event that deposits energy Ed in the detector results
in a pulse with an amplitude in dh about h. In gamma-ray spectroscopy,

g(h|Ed )
this spreading kernel has a shape similar to a Gaussian shape although,
in practice, it is usually skewed slightly towards lower amplitudes as a FWHM

consequence of different collection times of charge carriers produced in


different regions of the detector and the different amount of recombina-
tion and trapping they experience as they are collected. Shallow angle
Compton scattering also contributes slightly to this asymmetry. An ex-
ample of this amplitude kernel for a HPGe detector is shown in Fig. 20.1. h0 h
In effect, the detector systems that produce the voltage pulses operate on
the energy deposited Ed with an energy kernel z(Ed , E  ) that transforms Figure 20.1. A pulse-height spread-
Ed into a range of “apparent” energies E  , which are centered on Ed . The ing kernel for a HPGe detector as mea-
sured for the 1173-keV 60 Co gamma
resolution of a spectrometer is determined by the degree to which pulse ray [IEEE-325 1996]. Note the peak is
amplitudes are spread out around h0 or around Ed and is quantified by not quite symmetric about the centroid
the full width at half maximum (FWHM) either as a percent or in energy hmax .
units.
Often the amplitude spreading kernel is approximated by the Gaussian probability distribution
1
g(h|h0 , σ) = √ exp[−(h − h0 )2 /(2σ 2 )], (20.5)
2πσ
where h0 is the mean value or centroid and σ is the standard√ deviation. The peak value of the Gaussian
PDF occurs at the centroid
√ and is given by g max = 1/( 2πσ). As discussed in Sec. 6.8 the FWHM for a
Gaussian is FWHM = 2 2 ln 2σ  2.355σ.
It is worth noting that the energy resolution of semiconductor detectors is, in general, significantly better
than that for scintillation detectors or proportional counters. McGregor [2008] gives a good comparative
description of the resolution of various detector types. Each type of detector has its advantages and dis-
advantages. The chapters in this book on the various detector types provide useful information on the
characteristics of each type of detector.
The pulse heights are scaled to be within a finite interval [hmin , hmax ]. Typically, these limits are hmin = 0
and hmax = 10 V. In any case, the variables Ed and h are continuous variables. Whatever the pulse height
limits are, the response of a detector is typically binned into discrete “channels.” If n denotes an individual
discrete (integral) channel number and N is the total number of channels, then the channel width is
hmax − hmin
Δ= .
N
The channel numbers are related to the detected magnitudes of the voltage pulses (pulse heights) by the
relations

n = 1, if hmin < h ≤ hmin + Δ

= 2, if hmin + Δ < h ≤ hmin + 2Δ


..
.
= N, if hmin + (N − 1)Δ < h ≤ hmin + N Δ. (20.6)
1038 Radiation Measurements and Spectroscopy Chap. 20

Thus, the measured continuous pulse heights are converted into discrete channels and each pulse registers
a count in one and only one channel. NIM multichannel analyzer systems confine voltage signals or pulse
heights to be within 0–10 volts. Hence, a binary system may be subdivided with 2N voltage bins over
the 10-volt range. For N = 10, there are 1024 bins, or channels, over the 10 volt range having, in this
case, 9.8 × 10−3 volts per channel. Typical spectroscopic systems now often operate with N = 13 where
213 = 8, 192 channels, with some having N = 14, or 16,384 channels.
Although there are a finite number of discrete channels, corresponding to the pulse-height intervals
specified in Eq. (20.6), the peak centroid can occur at any continuous value of h. Thus, it is customary to
specify a linear relationship between the continuous values of h and a continuous channel number ñ, given
by
h − hmin
ñ = , (20.7)
Δ
which varies continuously between 0 and N . Henceforth, the term channel number is used to mean either
the discrete integer channel number n or the continuous channel number ñ; the context can be used to infer
the intent.1

20.3 Detector Response Models


Consider a source that emits photons at a rate with some energy distribution s(E) and a spectrometer
that detects the photons and produces a pulse-height spectrum. The basic spectroscopic relationship in its
continuous form can be written [Dunn and McGregor 2012],
 ∞
dR(h)
r(h) = = s(E)R(h|E)dE + b(h), h ∈ [hmin , hmax ], (20.8)
dh 0

where
• r(h) is the detector response such that r(h)dh is the expected number of counts within dh about h per
unit time.
• s(E) is the source strength, in photons per unit time, such that s(E)dE is the number of source photons
emitted within dE about E.
• R(h|E) is the detector response kernel such that R(h|E)dh gives the probability that a particle of energy
E interacting in the detector produces a pulse whose height is within dh about h. Here R(h|E) =
p(E, Ed )g(h|Ed ) where p(E, Ed )dEd is the probability that is a source gamma ray of energy E interacts
in the detector and deposits an energy in dEd about Ed in the detector.
• b(h) is the background count rate such that b(h)dh is the expected number of counts within dh about
h, per unit time, that are due to background radiation.
h
Note that R(h) = 0 r(h )dh is the cumulative number of counts per unit time due to pulses whose heights
h
are less than h and that R(h2 ) − R(h1 ) = h12 r(h)dh is the total number of counts, per unit time, whose
pulse heights are between h1 and h2 . Note also that R(h|E)dh accounts for the probability of transport of
source photons to and within the detector, deposition of energy Ed in the detector, and spreading of the
deposited energy into an apparent energy E  that produces a pulse whose pulse height is within dh about h.

1 Inthis book n is also used as a dependent variable that represents a net count rate n = c − b where c and b are the source and
background count rates, respectively. Likewise N refers sometimes to the total net counts, the number of spectral channels or
the number density of some particle. Again the context should make clear the meaning of n and N .
Sec. 20.3. Detector Response Models 1039

In general, a source can emit photons at J discrete energies and also over a continuum of energies. For
such sources
J
s(E) = sj δ(E − Ej ) + sc (E), (20.9)
j=1

where sj is the emission rate of photons of energy Ej from the source, δ(E − Ej ) is the Dirac delta function,
and sc (E) is the source emission rate of the photons with continuum of energies such that sc (E)dE is the
expected number of photons emitted within dE about E per unit time. For a detector that sorts counts into
discrete channels, one can substitute Eq. (20.9) into Eq. (20.8), integrate over each channel width, and write
the discrete form of the pulse height spectrum in the form


J  ∞
c(n) = sj Rn (Ej ) + sc (E)Rn (E)dE + bn , n = 1, 2, . . . , N, (20.10)
j=1 0

where c(n) is the number of counts recorded in channel n (per unit time), bn is the expected number of
counts recorded in channel n (per unit time) from background radiation, and Rn (E) is the detector response
function that is the probability that a particle of initial energy E that is emitted by the source produces a
count within the nth channel. Here
 nΔ
Rn (E) = R(h|E) dh.
(n−1)Δ

In general, spectra are accumulated over a counting time T , in order to increase the number of recorded
counts and, hence, improve the statistical precision of the measurements. In this chapter, it is assumed that
the source strength S(E) is constant in time. If the photon source is from the decay of a radionuclide, then
the measurement time T must be much less than the half-life of the radionuclide; otherwise, corrections must
be made to correct for the decrease in photon emission rate as was done in the discussion of foil activation
in Sec. 17.7.2.
The total counts obtained over counting time T per channel can be obtained by integrating Eq. (20.10)
over the counting time. The continuum source term can be due to photons emitted from the source over
a continuum of energies and/or to photons emitted at discrete energies from the source that scatter into
the detector from material around the detector. Because the primary objective of spectroscopy is to find
the Ej and sj , for j = 1, 2, . . . , J, it is customary to combine the continuum and background terms into a
generalized background. Doing so and integrating over the counting time T , one obtains


J
C(n) = Sj Rn (Ej ) + B(n), n = 1, 2, . . . , N, (20.11)
j=1

where C(n) ≡ Cn = c(n)T is the detector response in channel n, Sj = sj T , and


 ∞
B(n) = sc (E)Rn (E)dE + b(n) T. (20.12)
0

A plot of C(n) versus n is called a pulse height spectrum. Summation over any range of channels gives the
total counts within those channels.
1040 Radiation Measurements and Spectroscopy Chap. 20

(a)

Frequency C(E) Ei Ei+1 Energy


energy
(b) distribution
(c)

C(n i)
integral pulse
height spectrum
Counts

differential pulse
height spectrum

LLD Ei Ei+1 Energy Channel Number

Figure 20.2. Shown in (a) is the continuous energy distribution recorded with a radiation spec-
trometer. If a counter is connected to the detector, shown in (b) is the resulting count rate as a
function of the lower level discriminator setting, called the integral pulse height spectrum, super-
imposed on the radiation energy distribution. Shown in (c) is the resulting discrete differential
pulse height spectrum from (b).

Equation (20.11) describes an inverse problem, in which the specific Ej and Sj , j = 1, 2, . . . , J are sought
given J ≤ N measured pulse-height responses C(n). The generalized background Bn is typically not known
explicitly and, thus, further complicates the inversion process. There are different methods that can be used
to approach this inverse problem and the number M of channels, M ≤ N , used depends on the method
chosen. Because most spectrometers have thousands of channels, most spectroscopy inverse problems are
over-determined in the sense that there are considerably more responses available than unknowns.
It is noted that a variant of this inverse problem often is posed in terms of the k = 1, 2, . . . , K nuclides
present in a sample, each of which can emit photons at one or more discrete energies. Rather than look for
the J discrete energies and their intensities, one looks for the K nuclides and their concentrations. The form
of this inverse problem is similar to the form of Eq. (20.11) and is defined later more precisely by Eq. (20.95).

20.4 Gamma-Ray Spectroscopy


Suppose that the energy deposition in the detector is that shown in Fig. 20.2. A simple counter records events
in the detector that produced a signal exceeding the lower level discriminator (LLD). In the hypothetical
case with no electronic noise or background, all events interacting in the detector within measurement time T
are recorded if the LLD is set to zero. As the LLD is increased, those lower energy events in Fig. 20.2(a) are
excluded from the count rate, and the total number of recorded counts within time T decreases. This function
can be plotted as shown in Fig. 20.2(b), where the total integrated counts above the energy equivalent LLD
setting are plotted as a function of LLD setting. This plot is called the integral pulse height spectrum. There
are notable features in the integral pulse height curve that can be interpreted as follows. Flatter features
indicate energy regions where few events appear, usually from valleys in the energy spectrum. Steeper
features indicate energy regions where many counts are located and produce a large change in counts as a
function of LLD, often caused by energy maxima or peaks in the energy spectrum.
Sec. 20.4. Gamma-Ray Spectroscopy 1041

Although an experienced spectroscopist might be able to interpret the data of an integral pulse height
spectrum, it is usually the derivative of this spectrum that is used in spectroscopy, mainly because inter-
pretation is more straightforward. Suppose the energy spectrum of Fig. 20.2(b) is divided into n number of
channels, each channel having width of ΔE, then the total number of channels describing the spectrum is

n = (Emax − E0 )/ΔE, (20.13)

where Emax is the highest energy recorded as a function of channel number and E0 is an experimentally
determined zero offset. Ideally, the value of E0 is zero, but in practice usually is not. Suppose that each
energy bin is defined by the energies between two adjacent boundaries, i.e., by Ei+1 − Ei = ΔE. Then the
number of counts within each boundary, or channel n, is described by
 ∞  Ei  ∞  Ei+1
Ci = C(E)dE − C(E)dE − C(E)dE = C(E)dE. (20.14)
0 0 Ei+1 Ei

This result is the same as that found by taking the difference between the counts at Ei and Ei+1 in
Fig. 20.2(b). If this change in the recorded counts from the integral pulse height spectrum is plotted as
a function of the channel number (or energy), then a discrete differential pulse height spectrum is produced,

−(CEi+1 − CEi ) −ΔCounts


C(ni ) = = , (20.15)
Ei+1 − Ei ΔE

as depicted in Fig. 20.2(c).


Figure 20.2(c) is a histogram called the differential pulse height spectrum, which mimics the energy dis-
tribution seen by the detector, i.e., that of Fig. 20.2(a). For a good spectrometer, the measured energy
distribution is very similar to the actual distribution of energy deposited in the detector. However, for detec-
tors that have non-linear effects, recombination, or charge carrier trapping problems, the energy deposited
in the detector and the output signal are not necessarily proportional. Although a spectrum such as that
depicted in Fig. 20.2(c) can be developed with a single channel analyzer (Sec. 2.5.6) by sequentially moving
the energy window ΔE from zero up to 10 volts, it is a multichannel analyzer that is generally used to
display the energy spectrum (Sec. 2.5.13).

20.4.1 Gamma-Ray and X-Ray Spectral Features


Already discussed in Chapter 4 are the various ways that photons interact in a material and, for the present
application, in radiation detectors. The three main mechanisms are the photoelectric interaction, Compton
scattering, and pair production. Although Raleigh (coherent) scattering can be significant at low energies,
the photoelectric effect dominates (in the same energy region), usually by more than an order of magnitude.
Consequently, Rayleigh scattering is usually ignored in practical gamma-ray spectroscopy. Likewise, binding
effects become apparent only at low energies and are usually ignored.
Photoelectric Effect Features
Photons of relatively low energy (less than a few hundreds of keV) interact with the ambient medium mostly
through photoelectric absorption in which some of the photon energy is transferred to a photoelectron to
give it an energy
Tpe = Eγ − Eb , (20.16)
where Eb is the binding energy of the electron which depends on its electron shell of origin. The liberated
photoelectron moves through the detector medium causing more ionization through Coulombic interactions.
Ultimately, an average number of electrons per unit energy is liberated (or excited) in the detector medium.
1042 Radiation Measurements and Spectroscopy Chap. 20

- photoelectron
+
- +- -
C(E)

photopeak +
- -
g-ray +-++ K x-rays +
- photo-
+ electron

x-ray
-
+ - +-
escape
- -
+-++
peak
g-ray
- escapingK x-rays
E
Figure 20.3. A photoelectron absorbs the full gamma-ray energy, minus the binding
energy (hν − Eb ). This photoelectron produces free charges in the detector. Through
electron deexcitation, the binding energy is recovered by the emission and reabsorption
of characteristic x rays. Some x rays emitted near surfaces can escape the detector.
The resulting common spectral features are shown.

For scintillators, the important quantity is the average number of excited electrons that produce fluorescent
light. For gas detectors the important quantity is the average energy required to produce an electron-ion pair.
Similar to gas detectors, in a semiconductor it is the average energy required to produce an electron-hole
pair that is important. Ultimately, the number of information carriers is a function of the average energy w
required to produce the carriers and the absorbed photon energy. The effect is observed as a photopeak in
the differential pulse height spectrum (depicted in Fig. 20.3).
The binding energy Eb is recovered as electrons fall into lower energy levels. For instance, an ejected K
shell electron leaves an empty state, which can be filled by an electron falling from the L shell into the K
shell, producing a characteristic Kα x ray. The energy may also be recovered by the emission of an Auger
electron. If the x ray is absorbed by a lower energy bound electron (L or M ), it produces more ionization, and
the energy is recovered. The same is true for M shell electrons falling into K or L states, producing either
Kβ or Lα x rays, respectively. If generated near the detector surface, it is possible that these characteristic x
rays escape the detector, consequently causing the total deposited energy to be reduced by the characteristic
x ray energy. The photopeak under such a circumstance forms at the initial photon energy less the x-ray
energy, thereby creating an x ray escape peak as depicted in Fig. 20.3. This escape peak results primarily
from K shell x rays escaping and not from the loss of L shell x rays because L shell x rays have much lower
energies and are less likely to escape and, if they do escape, the lost energy usually blends with the main
photopeak and is less noticeable. These x ray escape peaks are a function of the detector material, and
appear mainly when (1) the detector is small so that a large fraction of the characteristic x rays can escape
and (2) when the detector is made of high Z material so that the characteristic x rays have larger energies.

Compton Scattering Features


At higher photon energies, ranging between tens of keV up to several MeV, depending on the material, the
Compton scattering effect becomes dominant compared to the photoelectric effect. The energy of a Compton
scattered electron is
Eγ2 (1 − cos θs )
Tcs = , (20.17)
me c2 + Eγ (1 − cos θs )

where θ is the photon scatter angle and me c2 = 511.0 keV is the rest-mass energy equivalent of an electron.
The scattered gamma rays have a continuum of energies from zero up to the maximum possible energy
Sec. 20.4. Gamma-Ray Spectroscopy 1043

-+ - Compton
- ++-
electron

+
- -
+-++
C(E)

g-ray
- - - Compton
+ + electron
Compton -+ - + -
edge
full energy reabsorbed -
- ++-
peak scattered photon +
- -
+-++
Compton Compton
continuum gap
multiple
g-ray
- escaping
scatters
scattered photon
E

Figure 20.4. Compton scattered electrons produce free charges in the detector up to
the maximum allowable energy transfer. If the Compton scattered photon is recaptured
and full energy deposited, the energy adds to the full energy peak. If the scattered
photon escapes the detector, the energy is added to the Compton continuum.

transfer to a Compton electron (for a single scatter at θs = π), namely


2Eγ2
Tcs = . (20.18)
me c2 + 2Eγ
A simple example is the case in which there is a single Compton scatter and the scattered gamma ray
escapes the detector. Under such a condition, the energy lost from the detector is given by Eq. (20.17).
Consequently, the pulse height spectrum is a continuum of energies from zero up to the energy described
by Eq. (20.18), termed the Compton continuum and is depicted in Fig. 20.4. The high energy limit of
the Compton continuum is called the Compton edge. If a considerable fraction of photons are Compton
scattered multiple times, ultimately terminating with photoelectric absorption, then the total initial photon
energy is represented by the energy peak in the pulse height spectrum. Because more than one type of
interaction contributed to the energy absorption, the proper term for this peak is the full energy peak. A gap
appears between the full energy peak and the Compton edge, termed the Compton gap. Multiple Compton
scatters that still result in some energy escaping the detector produce a small continuum in the Compton
gap. Ultimately, the Compton continuum is more prominent in small detectors than large detectors, mainly
because more Compton scattered photons escape the smaller detector.
Compton scattering of source photons in the surroundings and shielding of a detector can result in some
of these scattered photons reaching the detector and being absorbed in it. Theoretically, this backscatter
spectrum can have energies described by
Eγ me c2
Ebs = , (20.19)
me c2 + Eγ (1 − cos θ)
where θ is the scattering angle needed for the scattered photon to reach the detector. The minimum energy
of these scattered photons that reach the detector occurs when θ = π and is
Eγ me c2
Ebs = . (20.20)
me c2 + 2Eγ
Recall from Sec. 4.4.2 the discussion on scatter angle probability and photon energy, where forward scattering
becomes more probable with increasing gamma-ray energy. Hence, the differential backscatter cross section
1044 Radiation Measurements and Spectroscopy Chap. 20

actually decreases with higher gamma-ray energies (see Fig. 4.6). However, from Fig. 4.7, photons that
scatter with angle greater than about 100◦ emerge with nearly the same energies.
In practice, for geometrical reasons, it is unlikely that forward scattering in the surroundings or shielding
results in a significant number of scattered photons entering the detector. In fact, it is the larger scat-
tering angles that are most likely to return to the detector, so that the backscattering spectrum typically
increases at low energies in the pulse height spectrum. The effect is enhanced because low energy photons
are more readily absorbed in a detector than are high energy photons. Further, from Fig. 4.7, the energies
of backscattered photons are similar. A wide peak appears at the lower limit, called the backscatter peak, as
depicted in Fig. 20.5. This backscatter peak is actually a continuum with a somewhat discernible maxima.
Multiple scatters can cause the appearance of photon energies below the backscatter peak, but in practical
spectroscopy, these energy additions are difficult to distinguish from the Compton continuum.

shielding and surroundings


C(E)

full energy g-ray


peak
location
+ -
+ -
backscatter
backscattered
photons - + -
peak - +-
-
+ -+
multiple g-ray
scatters backscatter
continuum

Figure 20.5. Gamma rays that are Compton scattered in the materials surrounding
the detector may deposit energy in the detector. Consequently a backscatter spectrum
appears.

Pair Production Features


If the gamma-ray energy is greater than 1.022 MeV, then pair production is possible. When this photon
interaction occurs in a detector, 1.022 MeV of the photon energy is converted into the masses of the electron-
positron pair and the remaining energy shared as kinetic energy between the two particles. The particles
produce ionization in the detector just like photoelectrons and Compton electrons. After the electron loses
almost all its initial energy, it is absorbed in the material and returns to an allowed state. However, when
the positron comes to rest, it combines with an electron and annihilates, producing two 511-keV photons
emitted in opposite directions to preserve the zero linear momentum condition. If both of the annihilation
photons are reabsorbed in the detector, the initial gamma-ray energy is represented in the full energy peak.
If multiple events result in one 511-keV annihilation photon escaping the detector, then an energy peak
forms in the pulse height spectrum at Eγ − 511 keV, named a single escape peak. If multiple events result
in both 511-keV annihilation photons escaping the detector, then an energy peak forms in the pulse height
spectrum at Eγ − 1.022 MeV, named a double escape peak. Single and double escape peaks can be identified
by (1) noticing that no Compton edge forms and (2) noting their energy location with respect to the full
energy peak. Escape peaks are more prominent in small detectors than large detectors, mainly because a
larger fraction of annihilation photons escape the smaller detector.
Sec. 20.4. Gamma-Ray Spectroscopy 1045

electron
g-ray
-
- -++-
C(E)

escaping + +
double 511 keV photon
- -
escape single + +
peak escape
peak
full
energy
- +- -
+
peak
annihilation
+
- positron -+ -
-
+- ++
-
reabsorbed
511 keV photon
E
511 keV 511 keV

Figure 20.6. Gamma rays that undergo pair production produce energetic electron-
positron pairs. These particles produce free charge in the detector. When the positron
loses nearly all kinetic energy, it annihilates with an electron and emits two 511-keV
photons in opposite directions. Spectral features form accordingly if these annihilation
photons are reabsorbed, one escapes the detector, or if both escape the detector.

Pair Production and Fluorescence in the Surroundings


Pair production can also can occur in the shielding and surroundings, causing the emission of 511 keV
annihilation photons that can enter the detector and add to the pulse height spectrum (Fig. 20.7). Because of
this possibility of contamination, 511 keV annihilation photons are typically not used for efficiency calibration,
but can still be used for energy calibration.
The shielding and surrounding material, when irradiated by energetic photons, can also fluoresce by the
emission of characteristic x rays. These x rays appear in the pulse height spectrum at low energies, usually
below 90 keV. Because lead is a common shielding material, several energy lines ranging from 72.8 keV to
87.3 keV may appear in the low energy portion of the pulse height spectrum. Unless low energy spectroscopy
is required, usually these additional lines are of little consequence. However, directional shielding can be
applied to reduce the appearance of these lines, usually realized by a layer of copper placed between the
detector and lead shielding (as described further in Chapter 21).
Finally, bremsstrahlung fluorescence is generally present with gamma-ray detection. Many gamma-
ray emitting radioisotopes also emit beta particles, which in turn emit bremsstrahlung as they slow down
in a target material (Sec. 5.3.2). From Eq. (5.6), the energy intensity of bremsstrahlung increases with
target Z and the electron energy. A low Z beta-particle filter between the radionuclide source and the
detector can soften the bremsstrahlung spectrum. Also, photon interactions in the surroundings produce
energetic electrons, and these energetic electrons radiate bremsstrahlung as they slow down. Sample emission
distributions in lead are shown in Fig. 5.2. Although much of bremsstrahlung is self-absorbed in the shielding,
some of it can still interact in the detector. Because bremsstrahlung is generally featureless, this form of
fluorescent contamination increases the background but does not produce energy peaks. Regardless, the
addition of bremsstrahlung does increase the total counts in the pulse height spectrum, generally in the
lower energy channels, which can cause an overestimation of the gamma-ray flux.

Summary
To summarize, consider a radiation source that emits monoenergetic photons of energy Eo . A source photon
that enters the detector may experience any of several outcomes, including the following:
1046 Radiation Measurements and Spectroscopy Chap. 20

shielding and surroundings


C(E)

x-ray
g-ray
-+ -
full energy
peak
location + +
-- 511 keV
-
511 keV - -
+
+ -+
g-ray

x-ray -
- + positron
annihilation
E

escaping
511 keV photon

Figure 20.7. Gamma rays can also produce pair production in the surroundings. Con-
sequently, 511 keV annihilation photons can enter the detector from outside sources.
Energetic photons can also fluoresce the surroundings and the detector container to
produce x-rays that can enter the detector.

1. It may be completely absorbed by photoelectric absorption, in which case the deposited energy is the
photon energy, i.e., Ed = Eo .
2. It might undergo a sequence of one or more scatters within the detector and then be absorbed within
the detector by photoelectric absorption, which again leads to Ed = Eo .
3. It might scatter one or more times in the detector and then escape with an energy Er , which leads to
a deposited energy of Ed = Eo − Er .
4. If Eo > 1.022 MeV, it might undergo pair production in the detector, producing an electron-positron
pair that usually leads to the production of two 0.511-MeV photons by positron annihilation.2 If
both annihilation photons deposit all of their energy in the detector, then Ed = Eo . If one of the
annihilation photons escapes and the other is absorbed, the energy deposited is Ed = Eo − 0.511 MeV.
If both annihilation photons escape the detector, the deposited energy is Ed = Eo − 1.022 MeV. If
either or both annihilation photons scatter within the detector and then escape, an intermediate energy
within the range Eo − 1.022 < Ed < Eo is deposited.
5. It might not interact at all in the detector and so Ed = 0.
Note that outcomes 1 and 2 both contribute to a “full-energy” peak. Voltage pulses result whose pulse
heights are distributed from zero up to a maximum determined by the energy Ed and the energy resolution
of the detector. Thus a monoenergetic source produces a pulse-height spectrum that is distributed over the
many channels. The features shown in Fig. 20.3 through Fig. 20.6 can be combined to produce the expected
features that appear in a gamma-ray pulse height spectrum. Depicted in Fig. 20.8 are differential pulse
height spectra for monoenergetic gamma rays with energies below and above 1.022 MeV.

2 Positronannihilation occasionally takes place at higher than thermal energies. Consequently, annihilation photons of higher
energies are (infrequently) produced.
Sec. 20.4. Gamma-Ray Spectroscopy 1047

C(E)
full full
C(E)
(a) energy (b) energy
peak peak

backscatter
backscatter Compton peak double Compton
x-ray peak edge x-ray edge
escape single Compton
Compton peak gap
gap escape
511 peak
x-ray
x-ray keV escape
escape
peak
peak
Compton Compton
Compton
continuum continuum E
E
511 keV 511 keV

511 keV
Figure 20.8. Composite pulse height spectra for monoenergetic gamma rays formed from the
features shown in Fig. 20.3 - Fig. 20.6, with (a) Eγ < 1.022 MeV, and (b) with Eγ > 1.022 MeV.

An example pulse height spectrum obtained from a scintillation spectrometer exposed to the photons from
a 22 Na source, which emits 1.28-MeV photons and 0.511-MeV annihilation photons, is shown in Fig. 20.9.
The features in the spectrum, from right to left, include a full-energy peak centered about the channel
corresponding to E1 = 1.28 MeV, a Compton edge and a continuum extending from about channel 1250
downward, a full-energy peak due to 0.511-MeV annihilation photons, a Compton edge and Compton contin-
uum for the annihilation photons, and a backscatter peak. The maximum amount of energy that a photon
can give up in a Compton scatter occurs in a “backscatter” through an angle of π radians, and so the
Compton edge occurs over those channels that represent Compton scatters in the detector through angles
near π. Photons that are emitted by the source and backscatter (within either the source or the material
behind the source) have energies that are near the energy given by Compton scatter through π radians. The
backscatter peak in the spectrum of Fig. 20.9 is caused by source gamma rays that scatter, in or near the
sample, through angles close to π and then deposit full energy in the detector. This peak typically has a
FWHM that is larger than the FWHM of a full-energy peak for monoenergetic photons. The larger FWHM
occurs because source photons can backscatter in or near the source over a range of angles near π radians
and thus these scattered photons that reach the detector do not all have the same energy.
Summation Peaks
Other features that may appear in the pulse height spectrum are sum peaks, which are artifacts from two or
more photons interacting nearly simultaneously (i.e., within the resolving time) in the detector. Sum peaks
appear to be valid energies because they have many of the aforementioned features including Compton
edges and Compton gaps. Unknown energy peaks appearing in a pulse height spectrum can be checked to
determine if combinations of known energy emissions from the source sum to the unknown energy.
Given a source with multiple independent gamma-ray energy emissions Ei , each having intrinsic full
energy peak absorption efficiency of pi , the probability of N coincident photons leading to a full energy
absorption is represented by
)N
PN = KW (0◦ ) Ωf i pi Bi (20.21)
i

where Ωf i is the fractional solid angle for the source energy, Bi is the branching ratio (or frequency) of the
emission, and K is a geometric correction for parallax and detector shape, and W (0◦ ) is a factor included to
account for the angular correlation between the coincident gamma rays [Heath 1964; Rose 1953]. Gamma-ray
sources with multiple emissions per decay, such as 60 Co and 133 Ba, can be expected to develop sum peaks
1048 Radiation Measurements and Spectroscopy Chap. 20

Figure 20.9. The pulse height spectrum obtained by a NaI:Tl scintillation


detector exposed to a 22 Na source. The source emits photons at 0.511 MeV,
as a result of positron annihilations, and at 1.28 MeV, emitted as the product
22 Na transitions from the excited state to the ground state [McGregor 2008].

in the pulse height spectrum. Events of this type, in which two or more photons are released from a single
decay and are coincident in the detector, are often called true coincidences. The expected number of counts
in the sum peak are determined by multiplying the total source emission At by PN , where A is the source
activity and t is the counting time.
For geometries with a single point source and detector, the value of Ωf i is the same for all Ei . Consider
those cases in which there are only two simultaneous gamma-ray emissions such as occurs, for instance, with
60
Co. Then for a point source and single detector Eq. (20.21) becomes

P2 = KW (0◦ )Ω2f 1 2 B1 B2 . (20.22)

The parallax correction factor K approaches unity as the source-to-detector becomes large. Also, it is
often assumed that the emission directions of the different photons are uncorrelated so that W (0◦ ) = 1.3
Under these conditions the true coincidence sum rate for two simultaneous emissions reduces to the often
used expression
Rtrue = AΩ2f 1 2 B1 B2 . (20.23)
From Eqs. (20.21) and (20.23) it is clear that decreasing the fractional solid angle Ωf reduces the formation
of sum peaks more effectively than reducing counts in the real energy peaks because coincidences are a
function of ΩN
f while true energy peaks are proportional only to Ωf .
Sum peaks can also appear for high count rates, when two gamma rays from independent radioactive
decays are coincident within the processing time of the detection system. Recall from the discussion on
dead time coincidences in Sec. 7.3.2 that a random sequence of incoming pulses with average interaction rate
r. The average number of interactions within time t is simply rt. The Poisson distribution of Eq. (7.26)
describes the probability of multiple interactions in the detector within some time period t from a single

3 This assumption of course does not pertain to positron annihilation photons, which are emitted in opposite directions.
Sec. 20.4. Gamma-Ray Spectroscopy 1049

radiation source, namely,


(rt)n −rt
P(n|μ) = e , (20.24)
n!
where n is the number of interactions. If tr represents the pulse resolving time of the detector system, and
should these emissions enter a single detector within the pulse processing time, then they can produce a
coincidence sum peak. These events are sometimes referred to as accidental coincidences, mainly because of
the stochastic nature of radioactive decay allows such events to randomly occur by accident from unrelated
radioactive disintegrations. For a monoenergetic source, where the efficiencies, branching ratios, and solid
angles are the same, from Eq. (7.26) the probability that only one gamma ray interacts within the resolving
time of the same detector tr reduces to

P = P(1|μ) = rtr e−rtr . (20.25)

For small rt  1, Eq. (20.25) reduces to

P = rtr e−rtr  rtr (1 − rtr )  rtr = μ, (20.26)

which is also the average number of photons interacting in the detector within time tr . Suppose that an
initial gamma ray event occurs in the detector at t = 0, from gamma rays interacting at an average rate of
r. The rate of accidental coincidences, therefore, is the product of the average interaction rate r and the
average number of photons interacting within time tr

Racc = (r)(μ) = r 2 tr . (20.27)

Equation 20.27 is the widely used expression for accidental coincidences from a monoenergetic source [Vincent
1973].
There is a (smaller) possibility that two or more photons interact within the resolving time, which would
also reduce counts in the ideal spectrum without coincident effects. The probability that at least one event
occurs in time tr is given by
P = 1 − P(0|μ) = 1 − e−rtr , (20.28)
which yields a total accidental coincidence rate of

Racc = r(1 − e−rtr ). (20.29)

By adjusting (reducing) either r or tr , the rate of accidental coincidences can be reduced.


Shown in Fig. 20.10 is a spectrum of 60 Co emissions taken with an HPGe detector. The features include a
true coincidence sum peak from the two gamma-ray emissions along with two chance coincidence sum peaks
of the two emissions. Note that the counts in the 1173.2 keV + 1332.5 keV sum peak may be from both true
and chance coincidences, which are difficult to discern without some added analysis (e.g., with measurements
taken at different distances). Also shown in Fig. 20.10 are other features discussed in the previous sections,
including two Compton continua along with the coincidence sum Compton continua, single and double
escape peaks, 511-keV annihilation photons from the surroundings, Pb x rays, background from 40 K, and a
backscatter peak.
A consequence of summation peaks is their ultimate reduction in the counts represented in the actual full
energy peaks. Consider the sum peaks of Fig. 20.10. For each count in the sum peak formed from 1173.2 keV
+ 1332.5 keV gamma rays, one gamma ray each is removed from their corresponding real full energy peaks.
Also, the accidental sum peaks remove two gamma rays each from their corresponding full energy peaks.
One might correct the problem by simply adding the counts tallied in the sum peaks to the appropriate full
1050 Radiation Measurements and Spectroscopy Chap. 20

Figure 20.10. A gamma-ray spectrum of 60 Co taken with an HPGe detector. In-


cluded in the features are three sum peaks from true and chance coincident absorptions
of the 1173 and 1332 keV gamma rays. Courtesy of Nathaniel Edwards, KSU.

energy peak, yet this alone does not account for all coincident losses. The coincident absorptions where at
least one photon is Compton scattered produces a coincidence Compton spectrum below the sum peak(s).
Any coincidence of one photon with full energy deposition of a second photon alters the number of counts in
full energy peaks. For instance, a full energy absorption of one energy (say, E1 ) coincident with a Compton
scatter from another photon (E2 ) still removes a count from the full energy peak of E1 . Unfortunately,
these events fall into the coincidence Compton spectrum, and the original photon energies are difficult to
determine. Consequently, proper correction to the full energy peaks becomes difficult.
The total counts observed Coi in the full energy peak for Ei is related to the total counts Ci that should
appear in the peak by

Coi = Ci − (real coincident counts + accidental coincident counts), (20.30)

where the full energy of Ei is deposited in the detector for each coincidence. For conceptual simplicity,
consider a source with only two gamma ray emissions per decay, such as a 60 Co source. The observed counts
in the full energy peak for the gamma rays of energy E1 are represented by

Co1  At [Ωf 1 p1 B1 (1 − KΩf 2 I2 B2 − Attr (Ωf 1 I1 B1 ) − Attr (Ωf 2 I2 B2 ))] , (20.31)

where I2 is the total intrinsic counting efficiency of the second photon of energy E2 . For a single point
source and detector, the solid angle is the same, and the counts for E1 become

Co1  AtΩf p1 B1 [(1 − Ωf (KI2 B2 + Attr (I1 B1 + I2 B2 ))] . (20.32)

A similar expression can be found for the full energy peak of E2 . For decay schemes with more than two
gamma-ray emissions per decay, then the multiple coincident possibilities must be considered. These expres-
sions can become quite complicated as shown by Vincent [1975] and Smith [1978]. Byun et al. [2004] describe
a Monte Carlo method to obtain coincidence correction factors for multiple coincidences and detectors.
Sec. 20.4. Gamma-Ray Spectroscopy 1051

20.4.2 Spectral Response Function


A spectrum such as that in Fig. 20.9, normalized to unit concentration, is called the spectral response function
for a given radionuclide. Each nuclide has a characteristic spectral response function which is different for
each spectrometer for a specified source-detector geometry. Let the subscript k denote a specific nuclide.
Then the detector response function unk is the expected response (number of counts) of the spectrometer in
channel n per unit concentration of nuclide k.
Spectral response functions also can be associated with monoenergetic photons. If a source of monoener-
getic photons of energy Ej , in some specific source-detector geometry, irradiates a detector then the detector
response function unj gives the expected response in channel n per source particle of energy Ej emitted
from the source. In either case, it is not the full energy peaks that are of only interest; the entire spectrum
contains information about the source. Ways to exploit this dependence are considered later.

20.4.3 Qualitative Analysis


For some purposes, it is necessary to identify only whether or not a sample emits photons at certain discrete
energies Ej . This may be the case, for instance, if one wants to know if a sample contains a particular
radionuclide. Alternatively, a procedure such as EDXRF, NAA, or PGNAA can be used to excite charac-
teristic photons from a sample under investigation. If the element of interest is present, the characteristic
photons emitted from the sample should create full-energy peaks in a pulse-height spectrum collected from
the sample.
Photons of energy Ej that are emitted by the source produce full-energy pulses whose magnitudes are
distributed about a mean value of
hj = f −1 (Ej ). (20.33)
A pulse of magnitude hj produces a count in discrete channel nj if

hmin + (nj − 1)Δ < hj ≤ hmin + nj Δ.

For purposes of energy determination, it is useful to consider the continuous, non-integer, channel number nj
corresponding to the pulse-height hj of the full-energy peak. Then the gamma-ray energy can be estimated
by determining the continuous or fractional channel number ñj centroid of each peak.
It is then straightforward to obtain the corresponding hj from

hj = hmin + ñj Δ. (20.34)

For the usual case, where hmin = 0 and hmax = 10 V, this reduces to
10
hj = ñj . (20.35)
N
The expected source energy is then easily obtained from

Ej = f −1 (hj ). (20.36)

For a linear detector whose response is given by Eq. (20.2), then Eq. (20.36) is simply
hj − α
Ej = . (20.37)
β
If a nuclide emits several characteristic-energy photons, then one can gain confidence in the conclusion that
the element is present if peaks occur at all energies for which the photon abundance and the detection
efficiency would lead one to suspect that a peak should occur.
1052 Radiation Measurements and Spectroscopy Chap. 20

c(n)

Figure 20.11. An example of visual inspection to yield the channel numbers corre-
sponding to the centroids of two peaks in a spectrum. The vertical lines are used to
connect the apparent peaks to their centroid fractional channel numbers.

The simplest way to estimate the channel corresponding to the peak is by inspection of the plotted
spectrum. This technique often is adequate. One merely estimates the continuous channel number nj that
corresponds to the apparent centroid of the full-energy peak due to photons of energy Ej . For instance, in
the spectrum shown in Fig. 20.11, one can obtain estimates of the fractional channel numbers of the centroids
of the two peaks shown.4 It should be apparent that this procedure is subjective (different researchers may
estimate slightly different centroids) and, thus, has limited accuracy. Nevertheless this procedure may suffice
for some applications.
When estimation of the centroid by inspection is deemed insufficient, other methods must be employed.
The wavelet transform has been used in various spectroscopic applications, including nuclear magnetic res-
onance [Barache et al. 1997] and Raman spectroscopy [Xu et al. 1994]. However, this approach is not
commonly employed in gamma-ray spectroscopy and, thus, is not further considered here. Rather, it is
common that the centroids of the peaks present are identified as part of a fitting process that can determine
quantitative information about both the characteristic energies Ej and their relative abundances. Alterna-
tively, such methods may seek to identify particular radionuclides and their concentrations in a sample. Such
methods are discussed in the next sections.

20.4.4 Quantitative Analysis


The model of Eq. (20.11) identifies a general inverse problem in which many channels contain information
about the source distribution. One typically seeks to determine not only the characteristic energies Ej emit-
ted by the source but also the individual source strengths sj from the measured responses. Alternatively,
one may use the spectral responses to identify the nuclide k and its concentration ξk in a sample. Quanti-

4 Inthis example, the analyst is inexperienced because the maximum of a symmetric Gaussian distribution must lie between
the midpoint of the channel with the most counts and the channel boundary adjacent to the boundary with the second most
counts. Thus, both vertical lines should be moved slightly to the right.
Sec. 20.4. Gamma-Ray Spectroscopy 1053

tative analysis refers to the determination of quantities such as sj and ξk . There are several approaches to
quantitative analysis in spectroscopy, including the following:
1. Area under isolated peaks
2. Model fitting
3. Spectrum stripping
4. Library least-squares
5. Symbolic Monte Carlo

Summaries of how these methods are typically implemented are given in the following sections. In general,
one seeks to obtain both the Ej , j = 1, 2, . . . , J, and the net areas under each of the J peaks. For spectra
that are linearly related to the source strengths, the net area Aj under the jth full-energy peak is related to
Sj , the number of gamma rays emitted by the source during the counting time T , by

Aj
Sj = ,
ηj

where ηj is the detector efficiency, presumed known, at energy Ej ,


n2
Aj = [C(n) − B(n)], (20.38)
n1

and n1 and n2 are channel numbers over which the peak is spread. Similarly, in linear systems, the concen-
tration ξk of nuclide k is directly related to the net peak area.
A gamma-ray spectrum, generally, consists of a series of peaks atop a continuum produced by sources
emitting a continuum of energies and Compton plateaus from scattered photons. Ideally such a spectrum
can be described by a sum of K Gaussian peaks plus a continuum as


K
y(n) = gk (n, μk , σk ) + B(n), (20.39)
k=1

where
Ak
gk (ñ, μk , σk ) = √ exp[−(ñ − μk )2 /(2σk2 )], = Bk exp[−((ñ − μk )/τk )2 ]. (20.40)
2πσk
√ √
Here Ak = πτk Bk is the number of counts in peak k and σk = τk / 2 is the standard deviation of the
peak. Usually, the continuum is represented by a (piecewise) polynomial of ñ of low order. The principal
purpose of quantitative analysis of the spectrum is to determine values of Ak and μk from which radioisotope
identification and concentrations can be determined. Also in calibrated MCA spectrometer systems, the
continuous channel number ñ is replaced by the photon energy E and the channel number n by the energy
En at the channel midpoint.

20.4.5 Area Under an Isolated Peak


For isolated peaks, i.e., those that do not overlap with other peaks, a simple approach can be used to estimate
the net peak area. Generally, the peak is superimposed on a generalized background, as shown, for an ideal
1054 Radiation Measurements and Spectroscopy Chap. 20

case, in Fig. 20.12. To obtain the net area A, one identifies the channel numbers, n1 and n2 , at which the
peak disappears into the background. Then, the net peak area is estimated as


n2
C(n1 ) + C(n2 )
A= C(n) − (n2 − n1 ) . (20.41)
n=n1
2

The net area is the total number of counts between channels n1 and n2 minus the area under an (assumed)
linear background between C(n1 ) and C(n2 ). For instance, for the spectrum shown in Fig. 20.12, one might
choose n1 = 833 and n2 = 861. The total area between these channels is the sum of the counts in each
channel and the background is the area under the straight line connecting C(833) and C(861); thus, the net
area A is the area beneath the peak and above the background line in the figure.
This simple procedure cannot be applied to overlapping peaks and gives only approximate net areas
because the background may not be linear under the peak and identifying the channels n1 and n2 is subjective,
especially when the standard deviations of the responses, σ(C(n1 )) and σ(C(n2 )), are large relative to the
values C(n1 ) and C(n2 ).
C(n)

Figure 20.12. The net area A under the peak but above background.

20.4.6 Linear Least Squares Method for a Straight Line


Before methods to identify energy peaks and their corresponding energies, a review of the least squares
method to fit models to data is appropriate. The least squares method presented here and in subsequent
sections draws heavily on the discussion by Price et al. [2002].
Begin by considering the problem of fitting N data points (xi , yi ) to a straight-line model

y(x) ≡ y(x|a, b) = a + bx. (20.42)

This problem is often called linear regression by social scientists who invented the phrase a long time ago.
Here it is assumed that the standard deviation σi for the measurements yi are known and that the values of
Sec. 20.4. Gamma-Ray Spectroscopy 1055

xi are known exactly. To quantify how well this linear model agrees with the data, the chi-square statistic
is often used, which in this case is
N 
 2
yi − a − bxi
χ2 (a, b) = , (20.43)
i=1
σi

where σi is the standard deviation of yi and is assumed to be known. If the σi are not known, then simply
set σi = 1. If the measurement errors are normally distributed, as in counting data, then minimizing χ2
with respect to a and b gives the maximum likelihood estimators of a and b [Press et al. 1992]. Even if the
errors are not normally distributed the following approach is still useful.
At the minimum of Eq. (20.43) its derivatives with respect to a and b vanish, i.e.,

∂χ2 N
yi − a − bxi
0= = −2
∂a i=1
σi2
(20.44)
∂χ2  xi (yi − a − bxi )
N
0= = −2
∂b i=1
σi2

The equations can be rewritten more conveniently by first defining the following summations:

N
1 N
xi N
yi N
x2i N
xi yi
S≡ , Sx ≡ , Sy ≡ , Sxx ≡ , and S xy ≡ . (20.45)
σ2
i=1 i
σ2
i=1 i
σ2
i=1 i
σ
i=1 i
2
i=1
σi2

With these definitions, Eqs. (20.44) become

aS + bSx = Sy and aSx + bSxx = Sxy . (20.46)

The solution of these two equations for a and b is

Sxx Sy − Sx Sxy SSxy − Sx Sy


a= and b= , (20.47)
Δ Δ
where Δ ≡ SSxx − (Sx )2 .
This is not the end of the problem. The uncertainties in a and b must still be estimated because the
uncertainties in the measurements makes the above estimates of a and b also somewhat uncertain. Recall
from Sec. 6.9 that the variance in some function f of the yi is, for independent yi ,


N  2
∂f
σf2 = σi2 . (20.48)
i=1
∂yi

For the straight line the derivatives of a and b with respect to the yi are found from Eqs. (20.47)

∂a Sxx − Sx xi ∂b Sxi − Sx
= and = . (20.49)
∂yi σi2 Δ ∂yi σi2 Δ

Sum over the points as in Eq. (20.48) to obtain

σa2 = Sxx /Δ and σb2 = S/Δ. (20.50)


1056 Radiation Measurements and Spectroscopy Chap. 20

Finally, the covariance of a and b is covar(a, b) = −Sx /Δ from which the coefficient of correlation between
the uncertainty in a and b is
−Sx
ρab = √ , (20.51)
SSx x
which is a number between −1 and 1. A positive value of rab indicates that the errors in a and b are likely to
have the same sign, while a negative value indicates the errors are anti-correlated, i.e., the errors are likely
to have opposite signs.
Numerical Considerations
The formulas of Eqs. (20.47) are notoriously susceptible to roundoff error [Press et al. 1992]. To avoid
roundoff problems, define
  
N
1 Sx
ti = xi − , i = 1, 2, ..., N and Stt ≡ t2i . (20.52)
σi S i=1

Then, as can be verified by direct substitution into Eqs. (20.47)–(20.51),

1  ti y i
N
Sy − Sx b
a= and b= , (20.53)
Stt i=1 σi S
 
2 1 Sx2 1
σa = 1+ and σb2 = , (20.54)
S SStt Stt
Sx
cov(a, b) = − and rab = cov(a, b)σa σb . (20.55)
SStt
Application to Power and Exponential Functions
The linear least squares curve fit method can be used on power and exponential functions with appropriate
substitutions. For example, the function y(x) = αxβ can be curve fit by substituting Y = ln(y), X = ln(x),
a = ln(α), and b = β. Likewise an exponential function y(x) = αeβx can be fit to a straight line with
substitutions Y = ln(y), X = x, a = ln(α) and b = β. These substitutions can then be used to fit the linear
model
a + bX = Y (20.56)
to the observed data y(xi ) and xi , i = 1, . . . , N . The use of such a transformation to make a non-linear
model into a linear one is illustrated in Example 20.1.
Application to Unweighted Least Squares Fitting
Sometimes the uncertainties σi of the data points are unknown (such as in Example 20.1). In this case, an
unweighted straight line can be fit to the data by setting all the σi = 1. The values of a and b obtained from
Eq. (20.50) are then used to evaluate χ2 (a, b) from Eq. (20.43). The variances in the
 fit parameters are then
estimated by multiplying the values obtained from Eq. (20.54) (with σi = 1) by χ2 /(N − 2) [Price et al.
1992].

Example 20.1: An experiment is conducted with a set of lead absorbers of different thicknesses with a
137
Cs gamma-ray source which emits a 661.7-keV gamma ray. A spectrometer is used to measure the number
of counts per measurement acquired in the gamma-ray full energy peak as a function of absorber thickness.
Each measurement has the same counting time. Determine the linear and mass attenuation coefficients for
Pb for the gamma-ray energy emitted from 137 Cs.
Sec. 20.4. Gamma-Ray Spectroscopy 1057

Solution:
The data are best described by an exponential function,

y = αe−βx = αe−(β/ρ)(ρx) ,

where β is the linear attenuation coefficient in units of cm−1 and β/ρ is the mass attenuation coefficient in
units of cm2 g−1 . The absorbers were calibrated according to mass thickness ρx with units of g cm−2 . The
measured data are listed the following table.
137
Data for attenuation of Cs gamma rays through lead.

Mass Thickness Counts


(g cm−2 ) Xi2 in Peak Yi = ln yi Xi Yi
xi = Xi yi
0 0 10136 9.22385 0
0.9253 0.85618 8990 9.10387 8.4238
1.8213 3.31713 8290 9.02281 16.4332
2.6507 7.02621 7683 8.94677 23.7152
4.4936 20.19244 6184 8.72972 39.2279
7.1408 50.99102 4727 8.46105 60.4187

Sx = 17.032 Sxx = 82.3830 Sy = 53.4881 Sxy = 148.219

With S = N = 6 and all σi = 1, the set of linear fitting equations Eqs. (20.47) becomes

6a + 17.0322b = 53.4881 and 17.0322a + 82.3830b = 148.219,

which are easily solved to give


a = 9.2127 and b = −0.10560
With these values, the χ (a, b) of Eq. (20.43), with all σi = 1, is found to be χ2 = 8.516 × 10−4 . The
2

standard deviations of a and b are then


 estimated (as explained above) by multiplying the values obtained
from Eqs. (20.50), with all σi = 1, by χ2 /(N − 2). The results are

σa = 0.00927 and σb = 0.00257.

Converting back to an exponential α = ea = 10024 and β = b/ρ = −0.1056 ± 0.0026 so the best expected
fit to the data is
y = αe−βx = 10, 024(cts) exp[−0.1056(cm2 g−1 )ρx(g cm−2 )].
Hence, the mass attenuation coefficient at 661.7 keV is 0.1056 ± 0.00257 cm2 g−1 . Multiplication by the
mass density of lead of ρ = 11.34 g cm−3 , the linear attenuation coefficient at 661.7 keV is estimated to be
1.198 ± 0.029 cm−1 .

20.4.7 General Linear Least-Squares Model Fitting


Here is considered the problem of fitting a linear combination of M basis functions Xk (x) to a set of data
points (xi , yi ), i.e.,

M
y(x|a1 , ..., aM ) ≡ y(x|a) = am Xm (x), (20.57)
m=1
1058 Radiation Measurements and Spectroscopy Chap. 20

where Xm (x) can be highly non-linear in x. The term “linear” refers to the linear dependence of the model
on the parameters am . This problem is a more general problem of fitting a straight line to a set of data in
which X1 (x) = 1 and X2 (x) = x. As before, one seeks values of the parameters am that minimize the merit
function %M
N
yi − m=1 am Xm (xi )
2
2
χ = . (20.58)
i=1
σi
First define an N × M design matrix A with elements
Xj (xi )
Aij = . (20.59)
σi
In general N ≥ M because there must be at least as many data points as there are model parameters. Also
define a vector b with components
yi
bi = , i = 1, . . . , N (20.60)
σi
and a vector a whose components are the parameters am , m = 1, . . . , M .
The minimum of χ2 occurs when ∂χ2 /∂am = 0 or when

N
1 M
0= y i − aj Xj (xi ) Xm (xi ), m = 1, . . . , M. (20.61)
σ2
i=1 i j=1

This is a set of M linear algebraic equations in the M unknown am . These so-called normal equations can
be written compactly as

M
αmj aj = βm , m = 1, . . . , M, (20.62)
j=1

where 
N
Xj (xi )Xm (xi )
αmj = or equivalently α = AT · A (20.63)
i=1
σi2
and

N
yi Xm (xi )
βm = or equivalently β = AT · b. (20.64)
i=1
σi2
Equations (20.62) can be solved by any standard linear equation solver such as Gauss-Jordan or Cholesky
decomposition techniques. However, these normal equations are susceptible to roundoff errors and often
these simple solution methods fail and more sophisticated methods such as the singular value decomposition
technique should be used. Formally, the solution of Eq. (20.62) can be written as


M 
M 
N
yi Xm (xi )
aj = [α−1 ]jm βm = Cjm , (20.65)
m=1 m=1 i=1
σi2

where C = α−1 .
However, finding the model parameters is not the end of the data fitting problem. The standard errors
for the estimated parameters must also be estimated. With the usual formula for the propagation of errors
(see Eq. (6.75)) the variance of a fit parameter is estimated as


N  2
∂aj
σ 2 (aj ) = σi2 . (20.66)
i=1
∂yi
Sec. 20.4. Gamma-Ray Spectroscopy 1059

Because Cjm is independent of yi differentiation of Eq. (20.65) with respect to yi gives

∂aj M
= Cjm Xm (xi )/σi2 (20.67)
∂yi m=1

so that
 2
1  
M M N
∂aj
= C C
jm jk Xm (xi )Xk (xi ) . (20.68)
∂yi σi2 m=1 i=1
k=1
Substitution of Eq. (20.68) into Eq. (20.66) produces

M 
M 
N
Xm (xi )Xk (xi )
σ 2 (aj ) = Cjm Cjk = Cjj . (20.69)
m=1 i=1
σi2
k=1

The last simplification in this result arises because the term in square brackets is αkm (see Eq. (20.63)) and,
because α−1 = C, one has

M 
N
Xm (xi )Xk (xi ) 
M
−1
Cjk = Cjk Ckm = [C · C−1 ]jm = δjm . (20.70)
i=1
σi2
k=1 k=1

Hence the diagonal elements of the C matrix are the variances of the estimated parameters. Not surprisingly,
the off-diagonal elements of C are the covariances covar(aj , am ).
Computer programs and subroutines for performing linear least squares fits are provided by Press et al.
[1992], Bevington [1969] and Moré et al. [1980]. An application of this fitting procedure for an isolated peak
is given in the following example.

Example 20.2:
Consider a full-energy peak produced in a HPGe spectrometer from 350-keV gamma rays emitted by the
naturally occurring 214 Pb radionuclide. The measured data in the spectrum around this peak are listed in
Table 20.1. Fit the data to a Gaussian distribution and determine the area of the peak.

Table 20.1. A portion of a spectrum around the 351.93-keV 214 Pb full-energy


peak in the background spectrum shown in Fig. 21.7.

i Ei yi i Ei yi i Ei yi i Ei yi
(keV) cnts (keV) cnts (keV) cnts (keV) cnts
1 348.3 2626 9 350.4 2651 17 352.6 4927 25 354.8 2303
2 348.5 2574 10 350.7 2969 18 352.9 3561 26 355.1 2457
3 348.8 2594 11 351.0 3669 19 353.2 2888 27 355.3 2388
4 349.1 2588 12 351.3 4952 20 353.4 2461 28 355.6 2433
5 349.4 2558 13 351.5 6388 21 353.7 2417 29 355.9 2310
6 349.6 2579 14 351.8 7701 22 354.0 2399 30 356.2 2477
7 349.9 2658 15 352.1 7931 23 354.3 2550 31 356.4 2385
8 350.2 2650 16 352.4 6735 24 354.5 2405

Solution:
From Fig. 20.13 the data appears to consist of a single Gaussian on top of an almost linear background.
Thus, the general model of Eq. (20.39) reduces to
A
y(E, Eo , σ) = √ exp[−(E − Eo )2 /(2σ 2 )] + a1 + a2 E. (20.71)
2πσ
1060 Radiation Measurements and Spectroscopy Chap. 20

It is this model that is to be fitted to the data in Table 20.1. However, to use the general linear least-squares
fitting method described in this section, the peak energy Eo and its standard deviation σ must be known a
priori so that the fitting function depends only linearly on A, a1 and a2 .
Because the radioisotope is given as 214 Pb, then the energy of the decay gamma ray shown in Table 20.1
is Eo = 351.9 keV (see Appendix C), which, for this example is rounded to 520 keV. The variances of the
counts is taken as the number of counts, i.e., σi2 = yi . From past experience with the spectrometer used to
obtain the data of Table 20.1, the value of σ  0.47 keV. Thus, it is decided to look at two cases, one in
which σ = 0.45 keV and another in which σ = 0.50 keV. The results of the fits for the two choices of σ are
shown in Fig. 20.13. Clearly, σ = 0.50 kev is a better choice.

Figure 20.13. Two linear least-squares fit of Eq. (20.71) to the data


of Table 20.1 for two assumed values of σ.

To determine the number of counts in the peak, the method described in Sec. 20.4.5 could be used. By
inspection n1 = 9 and n2 = 20. Then the area is

20
area1 = c(n) − trapezoid area
n=9
1
= 56, 833 − [c(9) + c(20)][11] = 28, 717.
2

From the linear least squares fit (with Eo = 352 keV and σ = 0.50) it is found that A = 7161.79 ± 62.19
keV, a1 = 15819 ± 1316, and a2 = −37.75 ± 3.73 keV−1 . The energy width per channel is
E(31) − E(1)
ΔE = = 0.2700 keV/ch.
31 − 1
Thus, the least-squares area of the Gaussian peak is estimated as
7161.79 ± 62.188 keV
area2 = [A ± σ(A)]/ΔE = = 26, 525 ± 230.
0.2700 keV
Sec. 20.4. Gamma-Ray Spectroscopy 1061

20.4.8 Non-Linear Least-Squares Model Fitting


Often the model y(x|a) to be fitted to the data yi , i = 1, ..., N depends both linearly on some of the
parameters in a and non-linearly on the remaining M parameters. As before, in the least squares method,
values of the parameters are determined by choosing parameter values that minimize the merit function

N
yi − y(xi |a)
2
χ2 (a) = . (20.72)
i=1
σi

The normal equations (similar to Eq. (20.61)) are no longer linear in the parameters a and so cannot be
solved directly. Rather, iterative techniques must be used to find the minimum of χ2 (a).
Equation (20.72) describes a hypersurface in the M -dimensional hyperspace whose axes are the M pa-
rameters in a. One must incrementally traverse this hypersurface in some methodical fashion to find its
minimum. Such searches range from brute-force grid searches, in which one moves incrementally along each
axis to find a local minimum before searching along another axis, to more sophisticated searches, in which
each incremental step is taken in a direction opposite to the gradient of χ2 (a). However, the hypersurface of-
ten has many local minima in which an incremental search can become trapped and, thus miss the sought-for
global minimum. Moreover, these searches can often venture into regions of the hyperspace with physically
unrealistic parameter values, such as those producing negative Gaussian distributions. Such a problem is
frequently encountered if a search is begun far from the global minimum. Consequently, it is often necessary
to do a constrained search to prevent the search path from entering unrealistic regions of the hyperspace.
In the analysis of gamma-ray spectroscopic data (xi , yi ), xi is either the channel number n or the channel
midpoint energy En and yi is the measured number of counts in a channel. Typically, data in a gamma-ray
spectrum, or more often, a portion of the spectrum are fit to a sum of Gaussian peaks plus a polynomial to
represent the continuum upon which the peaks sit. For this case, the fitting model is


K  2
x − Ek
y(x|a) = Bk exp − + a0 + a1 x + a2 x2 + . . . + an xn . (20.73)
τk
k=1

The model parameters B1 , E1 , τ1 , ..., BK , EK , τK , a0 , a1, ..., an are the components of a. However, other
models are easily treated with the non-linear least squares technique described below.
Non-Linear Least-Squares Search
There are several ways to search the M dimensional hyperspace to find amin that minimizes χ2 (a) of
Eq. (20.72). Here the Leverberg-Marquardt (LM) method is presented and follows closely that presented
by Press et al. [1992]. Near the minimum of χ2 (a) the hypersurface should be well approximated by a
hyperparaboloid of the form
1
χ2 (a)  γ − d · a + a · D · a, (20.74)
2
where γ is a constant, d is an M component vector, and D is an M × M matrix. Take the gradient of this
expression and rearrange to obtain

a = D−1 · d − D−1 · ∇χ2 (a). (20.75)

At the minimum ∇χ2 (amin ) = 0, so amin = D−1 · d. Substitute this result into Eq. (20.75) to see that amin
can be reached from the current position in hyperspace acur in a single step as

amin = acur + D−1 · ∇χ2 (acur ). (20.76)


1062 Radiation Measurements and Spectroscopy Chap. 20

However, if Eq. (20.74) is a poor approximation, then the best that can be done is to step down the
gradient, i.e.,
anext = acur − constant × ∇χ2 (acur ) (20.77)
where the constant is sufficiently small to avoid overshooting the minimum. To use either Eq. (20.76)
or Eq. (20.77) of the above stepping procedures the gradient of χ2 (a) must be known for any a and to
use Eq. (20.76) one must also know D, the so-called Hessian matrix, whose components are the second
derivatives of χ2 (a).
The gradient of χ2 (a) with respect to the parameters a, which equals zero at the minimum of χ2 (a), is

∂χ2 N
[yi − y(xi |a)] ∂y(xi |a)
= −2 . (20.78)
∂am i=1
σi2 ∂am

Then differentiate this result to obtain the second derivatives, namely

∂ 2 χ2 N
1 ∂y(xi |a) ∂y(xi |a) ∂ 2 y(xi |a)
=2 2 − [yi − y(xi |a)] . (20.79)
∂am ∂al σ
i=1 i
∂am ∂al ∂al ∂am

Now define a vector β and matrix α as5


1 ∂χ2 1 ∂ 2 χ2
βm ≡ − and αml ≡ . (20.80)
2 ∂am 2 ∂am ∂al
Let δa = acur − anext , which is the next step in the search through hyperspace to find the minimum of χ2 (a).
If the iterative search is based on Eq. (20.76) with amin replaced by anext then manipulation of Eq. (20.76)
gives
D δa = ∇χ2 (a) or α δa = β, (20.81)
which can be rewritten as a set of linear algebraic equations

M
αml δal = βm . (20.82)
l=1

If, on the other hand, one wishes to use the steepest descent formula of Eq. (20.77) then
δal = constant × βl . (20.83)
The Hessian matrix of Eq. (20.79), in general, contains the second derivatives ∂ 2 y(xi |a)/∂al ∂am . These
terms can be ignored if they are zero (as in a linear model) or if they are small compared to the other terms.
Because the second derivatives are multiplied by [yi − y(xi |a)] a quantity that, for a good fitting model,
is the random measurement error. These errors can have either sign and should tend to cancel out when
averaged over all i. Further, the second derivatives can destabilize the iterative search for the minimum if
the spectrum is contaminated by outlier points. For these reasons, the second derivative terms in Eq. (20.79)
are almost always neglected. Additionally, their neglect makes the search somewhat simpler and, although
altering the matrix α changes the path taken in hyperspace to reach the minimum of χ2 (a), the values of
the parameters at the minimum are unaltered. Henceforth the elements of the α are taken as
N
1 ∂y(xi |a) ∂y(xi |a)
αml = 2 . (20.84)
σ
i=1 i
∂αm ∂αl

5 The α, which equals one-half of the Hessian matrix, is often called the curvature matrix.
Sec. 20.4. Gamma-Ray Spectroscopy 1063

The Levenberg-Marquardt Search


The Levenberg-Marquardt (LM) method is widely used for non-linear least-squares analyses. It varies
smoothly between the inverse-Hessian method of Eq. (20.82) when close to the minimum and the steepest
descent method of Eq. (20.83) when far from the minimum. The LM method is based on two key insights
made by Levenberg and Marquardt.
The first insight concerns the constant in Eq. (20.83). It is not dimensionless as is χ2 (a); but because βm
has dimensions of those of 1/am , which may be different for each m. Thus the constant of proportionality
between βm and δam must have dimensions of a2m . In the matrix α the only element with this dimension is
1/αmm , which defines the scale of the constant. However, this scale may produce too large a step size. To
reduce the step size, a factor λ 1 is introduced so that Eq. (20.83) can be written as

1
δal = βl or λαll δal = βl (20.85)
λαll

Clearly αll must be positive as is guaranteed by its definition in Eq. (20.84).


The second important key observation made by Marquardt is that Eqs. (20.85) and (20.82) can be
combined by defining a new matrix α as

αjj ≡ αjj (1 + λ) and αjm ≡ αjm , j = k, (20.86)

so Eqs. (20.85) and (20.82) can be replaced by the single equation


N
αml δal = βm . (20.87)
l=1

Notice that when λ is very large, α becomes diagonally dominant and Eq. (20.87) becomes Eq. (20.85). But
as λ becomes very small, Eq. (20.87) converges to Eq. (20.82).
Given an initial guess for the parameters a, the algorithm for the LM search for the minimum of χ2 (a)
proceeds as follows:

1. Compute χ2 (a).
2. Pick a modest value for λ, say λ = 0.001.
3. Solve Eqs. (20.87) for δa and evaluate χ2 (a + δa).
4. If χ2 (a + δa) ≥ χ2 (a), increase λ by a factor of 10 or other substantial amount. Then go to step 3.
5. If χ2 (a + δa) < χ2 (a), decrease λ by a factor of 10 and go back to step 3.

Continue this incremental walk through hyperspace until χ2 (a) decreases by a small amount such as 0.001
or some small fractional amount such as 0.001. Once an acceptable minimum has been found, the covariance
matrix
C = α−1 (20.88)
is computed (after setting λ = 1). The diagonal elements of this matrix give estimates of the variances of
the corresponding parameters.
In the examples below, the LM method is applied to the case of an isolated peak considered in Example
20.2 and to a case in which two peaks overlap. In both cases, the calculations use the LM computer
subroutines given by Press et al. [1992].
1064 Radiation Measurements and Spectroscopy Chap. 20

Isolated Peaks
To assure that the entire isolated peak is completely fit, it is suggested that the portion of the spectrum
extend to at least ±3σ above and below the centroid channel. These limits are chosen because the area
under a Gaussian over the range μ ± 3σ is 0.997 of the total area under the Gaussian and thus the parameter
A or B in Eqs. (20.39) and (20.40) is a very good approximation to the total area under the Gaussian.
For the portion of the spectrum containing an isolated peak, the appropriate fitting model y(x|a) is that
of Eq. (20.39) with K = 1 and a polynomial of low order n to describe the background upon which the peak
sits. The merit function to be minimized in this case is
N 2 N "  2 n # 2
yi − y(xi |a) 1 xi − μ
2
χ (a) = = yi − B exp − + m
am xi , (20.89)
i=1
σi σ2
i=1 i
τ m=0

where the components of the parameter vector a are B, μ, τ, a0 , ..., an . To use the LM method, the
derivatives of y(x|a) with respect to each parameter are needed. Here one has

dy(x|a) dy(x|a) 2(x − μ)


= f (x, μ, τ ), = Bf (x, μ, τ ) ,
dB dμ τ2
dy(x|a) 2(x − μ)2 dy(x|a)
= f (x, μ, τ ) , and = xj , j = 0, 1, ..., n. (20.90)
dτ τ3 daj
214
To illustrate this analysis approach, the data of Table 20.1 for a Pb peak are fit to a Gaussian plus a
linear function (n = 1) in Example 20.3.

Example 20.3:
For the portion of a spectrum containing an isolated peak, as given by the data in Table 20.1, the fitting
model y(x|a) is given by Eq. (20.73) with K = 1 and a linear background function so n = 1 in Eq. (20.73).
This is the same model used in Example 20.2, but now estimate the centroid of the peak and its standard
deviation by including them in the fitting parameters.

Solution:
The merit function to be minimized is that of Eq. (20.89) with n = 1. The initial guess of the parameter
values was

B = 3000 MeV, μ = 0.350 MeV, τ = 0.002 MeV, a0 = 1000, a1 = −200 MeV−1 .

After 23 LM steps through 5-dimensional parameter hyperspace, the χ2 (a) was reduced from an initial value
of 16,653 to 72.55, the minimum of χ2 (a). The best fit parameters at the χ2 (a) minimum were

B = 5583.6 ± 58.4, μ = 351.960 ± 0.0051 keV, τ = 0.74146 ± 0.00744 keV,


a0 = 14062 ± 1331 and a1 = −32823 ± 3776 MeV−1

The normalization of the Gaussian is A = πτ B = 7338.0±70.64 keV counts/channel, which, upon dividing
by the energy width per channel of 0.2700 keV/channel, gives the total counts in the peak as

A3 = 27, 178 ± 262.

This result is midway between the two estimates A1 = 28, 717√and A2 = 26, 525 ± 230 obtained in Example
20.2. Finally, the standard deviation of the peak is σ = τ / 2 = 0.52429 ± 0.00526 keV. The resulting
model fit and its two components are shown in Fig. 20.14. Of note is the estimated gamma-ray energy of
351.960 keV for this peak. This value compares very favorably to the accepted NUDAT value of 351.9321
Sec. 20.4. Gamma-Ray Spectroscopy 1065

Figure 20.14. The LM fit to the data of Table 20.1. Also shown


by dashed lines are the Gaussian peak component and the linear
background.

(18) keV. The small difference is easily accounted for by inevitable small errors in the energy calibration of
the channels of the spectrometer system.

Overlapping Peaks
Sometimes two or more peaks overlap. In situations where a peak is asymmetric or has a FWHM larger
than expected, one can try to fit multiple peaks to the data locally. In such cases, one might try a fitting
model of the form (see Eq. (20.39))


K  2
x − μj
y(x|a) = 2
Bj gj (x, μj , τj ) + a0 + a1 x + a2 x , where g(x, μj , τj ) = exp − (20.91)
j=1
τj

and K is the number of peaks one suspects might be overlapping.


Values of the model parameters a = (B1 , μ1 , τ1 , . . . , BK , μK , τK , a0 , a1 , a2 ) are found as those values that
minimize the merit function
N 2 N "
K  2 2 # 2
yi − y(xi |a) 1 xi − μk j
χ2 (a) = = y i − Bk exp − + a x
j i . (20.92)
i=1
σi σ2
i=1 i
τk j=0
k=1

As a practical matter, you might try K = 2 first and see if you obtain reasonable results. If not, try larger
values of K. Of course this model introduces new non-linear model parameters for each additional peak.
The fitting of multiple overlapping peaks, with asymmetric peak models, to XPS spectra is considered in
detail by Dunn and Dunn [1982].
Generally, the yi are either gross counts Ci in channel i or, for background-subtracted spectra, net
counts Ni in channel i. (Note that background subtraction removes only part of the generalized background,
the Bn of Eq. (20.12).) If the C(i) are gross counts, then one presumes that Poisson statistics apply and
σ 2 (yi )) ≡ σi2 = C(i). If the spectrum is background-subtracted, then σ 2 (yi ) = C(i) + Bi . If the C(i) result
1066 Radiation Measurements and Spectroscopy Chap. 20

from some other process, then one should use the appropriate variances in Eq. (20.92). For the non-linear
least-squares approach followed here, values of the model parameters a are chosen that minimize the merit
function χ2 (a). To use the LM minimization method, partial derivatives of χ2 (a) with respect to each
parameter are needed and for the above model are given by Eqs. (20.90).
An example of fitting two overlapping peaks is given in Example 20.4. In this example, and in many
non-linear least-squares fitting analyses, the incremental path through the χ2 (a) hypersurface may often
lead to physically unrealistic values of some of the parameters. This is particularly true for overlapping
peaks. Unless one starts the minimizing search with very good guesses for the μk for each peak, often a
broad positive Gaussian (B1 > 0) with a negative Gaussian (B2 < 0) results. Such is the case for Example
20.4. One way to avoid these unrealistic parameter values is to start the search very near the minimum of
χ2 (a), which is seldom known a priori, or to perform a constrained search along the hypersurface. In such a
constrained search, the current values of the parameters are examined after each step and, if outside some
preset range, an offending parameter is reset to the nearest range limit.

Example 20.4: Fit the model of Eq. (20.91) with K = 2 to the count data given in the table below.
Table 20.2. A portion of a spectrum giving channels and gross counts. The
data points (xi , yi ) to be fit are xi = i the channel number and yi = c(i) the
counts in channel i.
i C(i) i C(i) i C(i) i C(i)
117 2210 127 4756 137 45568 147 3827
118 2253 128 6176 138 36698 148 3416
119 2333 129 9761 139 23773 149 3156
120 2487 130 17016 140 14669 150 2896
121 2763 131 26462 141 10054 151 2713
122 2869 132 30846 142 7666 152 2448
123 2984 133 28392 143 6284 153 2335
124 3312 134 26822 144 5387 154 2119
125 3629 135 32667 145 4792 155 1957
126 4077 136 42618 146 4224 156 1754

Solution:
The LM method was used to find values of the best fit parameters. The derivatives needed for this method
are
dy(x|a) dy(x|a) 2(x − μi )
= f (x, μi , τi ), i = 1, 2 = Bf (x, μi , τi ) , i = 1, 2
dBi dμi τi2
dy(x|a) 2(x − μi )2 dy(x|a)
= f (x, μi , τi ) , i = 1, 2 = xj , j = 0, 1, 2. (20.93)
dτi τi3 daj

The search for the minimum of +χ2 (a) began with the following dimensionless starting values.

μ1 = 130. σ1 = 2.200 B1 = 22, 000. μ1 = 140. σ2 = 2.800 B2 = 38, 000.


a0 = −177000. a2 = 2680 a2 = −9.8400

After 15 steps, the initial value of χ2 (a) was reduced from 80,978. to 2034.92. Further iterations did not
change χ2 (a). Values of the best fit parameters are

μ1 = 131.664 ± 0.015 σ1 = 2.1298 ± 0.0157 B1 = 23, 403.4 ± 137.7


Sec. 20.4. Gamma-Ray Spectroscopy 1067

μ2 = 136.734 ± 0.0120 σ2 = 2.8700 ± 0.0138 B2 = 38538.5 ± 129.0


a0 = −166321. ± 1970. a1 = 2517.03 ± 29.22 a2 = −9.2409 ± 0.10771

The areas of the two Gaussians are


√ √
A1 = πτ1 B1 = 88348.1 ± 552.78 A2 = πτ2 B2 = 196039. ± 761.10

and the standard deviations of the peak are


√ √
σ1 = τ1 / 2 = 1.5060 ± 0.01108 σ1 = τ1 / 2 = 2.0295 ± 0.009724.

The fit function is shown in Fig. 20.15.


It is seen that the model fits the data quite well. One would expect that a good model would be within
the error intervals for about 68% of the data points and this seems to be the case here. The uncertainty in
each of the model parameters is small, relative to the parameter value, which also indicates a good fit. It
is noted that the values of i1 = 117 and i2 = 156 are well beyond the 3σ range for the σ1 and σ2 obtained.
Thus, the A1 and A2 values should be good estimates of the net areas under the two peaks.

Figure 20.15. A fit of two overlapping peaks with a quadratic


 background.
The solid line is a weighted least-squares fit with σi = c(i) and the dotted
line is an unweighted least-squares fit with σi = 1.

20.4.9 Spectrum Stripping


If response functions can be collected or generated for all the sources (or radionuclides) that are expected
to be present in an unknown sample, and if the dependence of the response model is linearly related to the
source strengths or radionuclide concentrations, then the method of spectrum stripping can be applied. This
procedure is as follows:
• Collect a spectrum from the unknown sample.
1068 Radiation Measurements and Spectroscopy Chap. 20

• Identify the highest-energy peak in the spectrum.

• Subtract the response function for that energy peak, weighted by a constant, such that the peak is
effectively removed.

• Proceed down the spectrum while subtracting other weighted response functions until all peaks are
removed.
If the residuals are randomly distributed about zero or about some smooth background, then the specific
response functions stripped from the spectrum for the unknown identify the radionuclides present and the
weighting constants estimate the source strength or concentration of each radionuclide.

20.4.10 Library Least-Squares


Because a detector produces a spectrum, even for a monoenergetic input one can try to utilize the entire
spectral response, or at least a significant part of it, rather than just the response values near each peak or set
of overlapping peaks. The library least-squares approach, originally introduced by Marshall and Zumberge
[1989], asks the following question. Why focus on only the peaks since other parts of the spectrum also
contain information related to the abundances of the radionuclides that produce the peaks? One approach
for using all of the information in a spectrum is the library least-squares (LLS) method, as implemented, for
instance, by Gardner and Sood [2004] and Gardner and Xu [2009]. The LLS method is based on a library
that contains detector response functions for all radionuclides that might possibly be present in the sample
whose spectrum is to be analyzed in order to determine the abundances of specific radionuclides. Then some
fitting technique, such as least-squares or weighted least-squares, is used to fit the library spectra to the
spectrum from a sample whose radionuclide abundances are sought.
This approach was not possible many years ago because one could not experimentally measure good
spectra from all candidate radionuclides or a sufficient number of monoenergetic gamma rays. However,
Monte Carlo modeling has become sufficiently robust that detector response functions can be calculated for
almost any radionuclide. When Monte Carlo is used to generate detector response functions, the method often
is referred to as Monte Carlo library least-squares or MCLLS. In this method, one calculates monoenergetic
detector response functions Rn (E) for a wide range of discrete energies that can be emitted by sources
of interest. Examples of such MC calculated detector response functions are shown in Fig. 20.16 and were
calculated by special MC software and empirical resolution functions [Gardner and Sood 2004]. The response
function Rn (E) is the probability that a photon of energy E emitted by the source produces a count in
channel n. This response function, as before, includes the probability a source photon reaches the detector,
a probability which depends on the specific source-detector geometry but it, generally, does not include
photons scattered into the detector by material around the detector, i.e., so-called roomshine.
To determine the concentrations of various radioisotopes present in a sample, response functions, per unit
activity concentration, for each possible radioisotope likely to be in the sample must first be constructed.
A library of such radioisotopic response functions Rkn can be constructed from the monoenergetic response
functions Rn (E), for a given source-detector geometry, as


I
Rkn = fik Rn (Eik )ξˆk , (20.94)
i=1

where fik is the frequency a photon of energy Eik , i = 1, ..., I is emitted per decay of radionuclide k and ξˆk
is the decay rate of a unit activity concentration of the radionuclide.
Sec. 20.4. Gamma-Ray Spectroscopy 1069

Figure 20.16. Examples of library response functions Rn (E) for a 6 in × 6 in cylindrical


NaI detector for monoenergetic photons normally and uniformly incident on the circular
end of the crystal. No contribution from scattering in material around the detector is
included as indicated by the absence of backscatter and annihilation peaks although
several annihilation escape peaks from the crystal are evident. These response functions
are a small part of the library for a 512-channel spectrum over the photon range 0–11.38
MeV. Courtesy of Robin Gardner, NCSU.

Then the expected number of counts y(n) recorded in channel n in a measurement time T produced by
a sample of K possible radioisotopes is


K
y(n|ξ) = T Rkn ξk , n = 1, ..., N, (20.95)
k=1

where ξk are the radioisotopic activity concentrations being sought. Again it is assumed all the activity
concentrations remain constant over the measurement time T . If C(n) are the observed number of counts
in channel n from the sample, then the vector ξ, whose components are the concentrations ξk , can be
determined as those values that minimize the merit function

N
χ2 (ξ) = Wn [c(n) − y(n, |ξ)]2 , (20.96)
n=1

where Wn is a weight factor, often taken as Wn = 1/σ 2 (C(n)) = C(n). Because the response functions do
not include background and roomshine, the counts C(n) must first be corrected for these contributions. If a
fitted ξk value is negative or near zero for one or more k, then the corresponding radionuclides might not be
present in the sample. In this case, it is a good practice to remove the detector response functions for these
radionuclides and repeat the analysis to see if a good fit is obtained.
The process just described assumes the response model is linear in the radionuclide concentrations and,
thus, can be referred to as the linear LLS approach. This approach is very similar to the previous linear
1070 Radiation Measurements and Spectroscopy Chap. 20

weighted least-squares process used to fit Gaussian distributions to spectral peaks. But here more features
of the spectrum other than just the full-energy peaks are used. There are instances, however, in which
the model is not linear in the radionuclide concentrations. Such cases arise in prompt gamma-ray neutron
activation analysis (PGNAA) and energy dispersive x-ray fluorescence spectroscopy (EDXRF).
Non-Linear Spectra
Generally, the samples used in a neutron activation analysis (NAA) are small and their mass can be accurately
measured and, because one is usually seeking concentrations of trace elements, a NAA analysis is well
approximated as a linear process and application of linear LS technique is appropriate. However, for bulk
samples, a prompt-gamma neutron activation analysis (PGNAA) is non-linear, primarily for the following
reasons:

• Sample mass, which often is not known, affects the flux density and the macroscopic capture cross
section of the sample.

• The composition of the sample, which is unknown in advance, affects the spectrum. In particular,
moisture content strongly affects the thermal-neutron flux density, which is what gives rise to the
prompt gamma rays. Also, neutron absorbers affect the thermal flux density.

Thus, non-linear models are needed for a PGNAA. Such models are iterative in nature and require the
need to calculate spectral responses. Usually, Monte Carlo methods are used for such calculations. The
general Monte Carlo Library Least-Squares (MCLLS) approach in the non-linear case proceeds as follows.

1. Assume values for the concentrations and use Monte Carlo to generate a complete spectrum for a
sample of this assumed composition.

2. Keep track of the individual spectral responses for each element within the Monte Carlo code, so as to
provide library spectra unk for each radionuclide.

3. Use linear LLS to estimate the radionuclide concentrations ξk , k = 1, 2, . . . , K from the sample spec-
trum.

4. If the calculated ξk , k = 1, 2, . . . , K match the assumed composition closely enough, you are done. If
not, pick a new composition, based on the calculated concentrations, and repeat the process.

5. Iterate until you converge to the actual composition, to within a desired tolerance.

Results of this general procedure are given, for instance, by Gardner and Xu [2009].

20.4.11 Symbolic Monte Carlo


In X-ray fluorescence, the responses are due to the elements present, but each element is composed of ra-
dionuclides and the convention was introduced earlier to refer only to radionuclides. Hence in the discussion
below, elemental concentrations are called nuclide concentrations. Non-linear matrix effects lead to absorp-
tion and enhancement in EDXRF. For instance, the characteristic x rays of nuclide a can be absorbed by
elements with lower atomic numbers, which reduces the signal from nuclide a and enhances the signals for
the lower atomic number nuclides. This effect means that the models in EDXRF also are not linear in
the nuclide concentrations. Another implementation of Monte Carlo has been used in the EDXRF case.
The method, originally called Inverse Monte Carlo (IMC) [Dunn 1981], was applied to EDXRF by Yacout
and Dunn [1987] for primary and secondary x rays. Mickael [1991] extended the work to include tertiary
fluorescence.
Sec. 20.5. Radiation Spectroscopy Measurements 1071

The term IMC has been used for other purposes, e.g. to solve inverse problems by iterative Monte
Carlo simulations in which the unknown parameters are varied until simulated and measured results agree
sufficiently. The acronym IMC also has been used for “implicit Monte Carlo” [Gentile 2001]. Thus, Dunn
and Shultis [2009] recently proposed renaming the version of IMC that is non-iterative in the Monte Carlo
simulations symbolic Monte Carlo (SMC) because the method proceeds by using symbols in the Monte Carlo
scores for the unknown parameters.
SMC is a specialized technique in which the inverse problem of estimating the k and ξk is solved by a
system of algebraic equations generated by a single Monte Carlo simulation. For purposes of illustration, a
ternary system (one that contains three elemental nuclides) is considered. In essence, SMC creates models,
with symbols for the unknown concentrations ξk , for the areas under all of the various x-ray peaks (e.g., Kα
and Kβ ) in a single simulation. The models depend on the detector efficiency as a function of energy, the
nuclide concentrations, the primary, secondary, and tertiary fluorescence produced in the sample, and the
background. For a ternary system, three equations result. The equations are rather complex (see Yacout
and Dunn [1987] and Mickael [1991]) but can be developed using only a single Monte Carlo simulation.
The advantage of this approach is that there is no need to iteratively run full Monte Carlo simulations as
the assumed concentrations are varied. The disadvantage is that development of the model is involved and
the algebraic equations are quite complex. Nevertheless, the method has been shown to work well in x-ray
spectroscopy and can, in principle, be applied to other spectroscopic applications, such as PGNAA, in which
the responses are non-linear functions of the concentrations.

20.5 Radiation Spectroscopy Measurements


The purpose of radiation spectroscopy is to identify energetic emissions from radioactive materials. Such
emissions are reported with several metrics, mainly the confidence in the identified energy or the energy
resolution and the source activity (a function of the detector efficiency). The choice of detector is determined
by the application and required spectroscopic performance. Detectors needed for field applications with
sufficient spectroscopic performance to identify common isotopes may be best performed with lower resolution
scintillation detectors. Measurements requiring high resolution spectroscopy generally require more expensive
semiconductor spectrometers. No matter the type of spectrometer, it must undergo an energy calibration
before any measurements can be made.

20.5.1 Channel Calibration


Calibration of the spectrometer channels in energy units is relatively simple, particularly if a linear en-
ergy/channel response is assumed. Typically two particle energies are chosen with relatively wide separation.
For instance, 60 Co and 57 Co might be chosen. The peak channel ñH for the higher energy EH and the peak
channel ñL for the lower energy EL are observed and a simple linear fit between these two channels provides
a channel energy calibration, i.e.,
 
EH − EL
E(ñ) = ñ + E0 , (20.97)
ñH − ñL
where E0 is the energy offset at channel ñ = 0.0, which is found from
 
EH − EL
E0 = EH − ñH . (20.98)
ñH − ñL

For simplicity, the continuous ñ is often taken as the channel number n which equals ñ at the midpoint
of a channel. The term in parentheses in the above equations is the energy width per channel ΔE and is
1072 Radiation Measurements and Spectroscopy Chap. 20

an important spectrometer parameter because it defines the minimum energy resolution possible with the
spectrometer.
Semiconductor materials usually show good signal linearity with energy deposition, but there are many
scintillators that exhibit a non-linear output with energy, especially at lower energies (see Sec. 13.2.2).
Example scintillators include NaI:Tl and CsI:Tl in the energy region below 500 keV. For such non-linear
detectors, several energies in the non-linear region should be used to fit a polynomial function to the channel
energy calibration.

20.5.2 Quality Metrics


Several quality metrics have been established, some official and others less so, that depend on the system and
type of detector. These metrics are used to give the user an idea of the expected detector performance under
different measurement conditions. Metrics include measurements of detection efficiency, energy resolution,
channel width corrections, figure of merit, noise resolution, energy rate limit, and peak-to-Compton ratio.
Many of these metrics are described in the IEEE Std 325-1996 document for HPGe detectors, outlined in
this section.
Detection Efficiency
There are multiple methods for defining and measuring the efficiency of a gamma-ray spectrometer. The
efficiencies of most interest and utility are the absolute efficiency, the intrinsic efficiency, and the escape
peak efficiency. In Sec. 7.1 a general description of detector efficiencies was given. Here efficiencies for a full
energy peak from a gamma-ray spectrometer are defined.
Total Intrinsic Detection Efficiency The total intrinsic detection efficiency is defined by


N
Asp
I = (20.99)
i
AΩf tBi

where Asp are the recorded counts from the entire detector spectrum, t is the live time of the counts, A
is the source activity, Ωf is the fractional solid angle subtended by the detector, and Bi are the branching
ratios of the radiation emissions. For instance, 60 Co emits two gamma rays per decay (B = 2), while only
85% of decays from 137 Cs result in the emission of a 661.7 keV gamma ray (B = 0.85). This metric I
yields some information about the overall detector counting efficiency, but does not give information on the
energy resolution performance. Further, this particular metric is subject to changes with the LLD setting,
and background contamination can skew the results.
Intrinsic Peak Efficiency The intrinsic full energy peak efficiency, described in Sec. 7.1 and repeated here
for convenience, is defined by
Ap
peak = (20.100)
AΩf Bt
where Ap are the recorded counts from the detector in the full energy peak, t is the live time of the counts,
A is the source activity, Ωf is the fractional solid angle subtended by the detector, and B is the branching
ratio of the emission under investigation. The intrinsic peak efficiency is similar to the intrinsic detection
efficiency, except the Ap pertains only to those counts located in the background subtracted full energy
peak. It is notable that the intrinsic peak efficiency may be difficult to determine accurately for several
detector types. For instance, the size and shape of an HPGe detector may be difficult to assess because the
actual crystal is much smaller than the apparent cryogenic packaging (see Fig. 16.34). A similar situation
exists with scintillation counters whose crystal is hermetically packed in a light-tight reflecting cannister.
The practical outcome of the intrinsic peak efficiency is a function of the packing cannister, the absorbing
Sec. 20.5. Radiation Spectroscopy Measurements 1073


   


    


   
 
Figure 20.17. Measured intrinsic peak efficiency for a 25% relative efficient n-type HPGe
detector. The sources used for the calibration were 241 Am, 133 Ba, 152 Eu, 137 Cs, 60 Co,
188 Ta, 56 Co, 49 Ti, and 36 Cl. Data acquired from Kis et al. [1998].

material (NaI:Tl, HPGe, CdTe, etc.), the type of electrical contacts, the detector size, and the detector shape.
Energy absorption in the detector encapsulation and contact dead layer affect the low energy efficiency, while
the atomic number and volume of the detector determine the high energy efficiency (see Fig. 16.35). An
example of the efficiency variation is shown in Fig. 20.17 for a 25% relative efficient, bulletized coaxial n-type
HPGe detector [Kis et al. 1998].
A variety of gamma-ray sources can be used to measure the intrinsic peak efficiency over the energy
region of interest. Afterwards, a curve fit can be used as a predictive measure of efficiencies at other energies
within the measured span [Kis et al. 1998]. Although there are several curve fitting functions offered in the
literature, many examples listed in Kis et al. [1998], modern commercial curve fitting computer programs
are available that can provide high fit r2 values (> 0.999).
Escape Peak Efficiency The escape-peak efficiency, mainly the single and double escape peaks from pair
production, is a measure of the detector’s ability to effectively recapture 511-keV annihilation photons.
Larger escape peaks are indicative of larger losses. Although there are multiple definitions of this metric
in the literature, a generally accepted definition for the intrinsic escape peak efficiency is that described by
Cline [1968] and Nafee [2011],
Aep
es = , (20.101)
AΩf Bt
where Aep pertains to the number of counts in either the single escape peak or the double escape peak. To
determine the number of counts in either escape peak, the subtraction method of Eq. (20.41) is employed.
Equation 20.101 can be rewritten as
Aep
es = peak , (20.102)
Ap
where the escape peak under investigation is for the corresponding full energy peak.
1074 Radiation Measurements and Spectroscopy Chap. 20

Figure 20.18. Spectral calibration and features for the 60 Co 1332.5-keV full energy peak
taken with a HPGe detector. The left axis is for the full energy peak and the right axis
is for the tails and the background subtracted data on either side of the peak. The open
circles are measured counts C(n) and the solid circles are counts corrected for background,
i.e., N (n) = C(n) − B(n). Adopted from IEEE 325-1996.

It is notable that escape peaks can be used to identify the initial gamma-ray energies. Escape peaks do
not have a Compton gap or Compton edge, and the apparent lack of these features can assist with their
identification. Although gamma rays equal to or greater than 1.022 MeV can be absorbed through pair
production, escape peaks usually do not become apparent for gamma-ray energies below approximately 1.5
MeV.

Energy Resolution
A method to determine the energy resolution of a gamma-ray spectrometer is prescribed by the IEEE Std
325-1996 and was developed for a HPGe detector and a 60 Co check source. The method, which appears
to be used by few if any researchers, makes no use of statistical uncertainties in the spectral count data
(unlike the weighted least squares fitting methods used earlier). Rather it depends on a very high number of
counts in the full energy peak so statistical uncertainties are of little consequence. The one unique feature
of this standard, however, is that the method makes no Gaussian symmetry assumption about the shape
of the full energy peak and it is capable of treating asymmetric peaks that are wider at energies below the
peak energy than above—a feature observed in many spectrometers. In essence, the method relies solely on
manipulations of the observed channel counts C(n) ≡ Cn to estimate the FWHM.
The IEEE Std 325-1996 recommends a 8192 (213 ) channel multichannel analyzer with the 1332.5-keV
60
Co full energy-peak scaled to appear in channel 4032. The reason for the location is to ensure that at least
5 channels are included within the FWHM of the energy peak. If the detector under test has worse resolution
than normally expected from a HPGe detector, a lower channel can be used provided that the 5 channel
criteria is maintained (see Fig. 20.18). At least 10,000 counts must appear in peak maximum channel, and
the spectrum and live time are to be recorded. If a pulse generator is used to measure electronic noise, the
pulser peak is to be set between the 60 Co energy peaks (1173.2 keV and 1332.5 keV), and as close as possible
to the 1332.5-keV full energy peak without interfering with the recorded counts. The method does allow for
other gamma-ray sources, but the requirement that at least 5 channels be included in the FWHM remains.
Sec. 20.5. Radiation Spectroscopy Measurements 1075

Begin by identifying the first channel nL to the left of the peak which shows no contribution from the peak
and consists solely of background events. Likewise identify nR the first channel above the peak that shows no
peak contribution. Then average the 6-8 channels below nL and above nR to find the average background BL
immediately below the peak and BR above the peak. Use a linear equation between (nL , BL ) and (nR , BR )
to represent the background under the full peak, i.e.,
BL − BR
B(n) = BL − (n − nL ) , nL ≤ n ≤ nR . (20.103)
nR − nL
The net peak counts corrected for background are then N (n) = C(n) − B(n).
As shown in Fig. 20.18 the channels containing the seven highest counts are identified with the letters
A, B, C, D, E, F, and P and the counts in these channels are used to characterize the peak. The peak may
not be exactly at the centroid of channel nP , which occurs only if NE = NF , and may be slightly shifted to
ñmax where the peak has the true maximum Nmax . To determine the true maximum fit, the three highest
counts to the parabola
N (ñ) = αñ2 + β ñ + γ. (20.104)
The maximum count Nmax occurs when dN (ñ)/dñ = 0 or at ñmax = −β/(2α). The maximum is found
to occur at
(NE − NF )/2
ñmax = nP + , (20.105)
NE + NF − 2NP
where NE ≡ N (nE ) and so on for the other peak channels. The maximum number of counts is

(NE − NF )2
Nmax = NP − . (20.106)
8(NE + NF − 2NP )

The FWHM maximum can be measured by producing linear extrapolations for the data points that
straddle the FWHM location at a height Nmax /2. This procedure is performed after the background has
been subtracted. For example from Fig. 20.18, these extrapolations would be applied to data points at
positions A and B and also at positions C and D. Note nB − nA = nC − nD = 1. Thus, the location ñl
between A and B of the left end of the horizontal FWHM line is found to be
Nmax /2 − NA
ñl = nA + . (20.107)
NB − NA
Similarly the right end ñr between C and D is

Nmax /2 − NC
ñr = nC − . (20.108)
NC − ND
The difference between these two limits then gives the FWHM in channels, namely

NC − Nmax /2 Nmax /2 − NA
FWHMch = ñr − ñl = (nC − nA ) + − . (20.109)
NC − ND NB − NA
The energy resolution in energy units and as a percent are
ΔE
FWHMenergy = ΔE FWHMch and FWHM% = 100 FWHMch , (20.110)

where ΔE is the channel width in energy units (typically keV) and Eγ is the energy of the gamma ray.
1076 Radiation Measurements and Spectroscopy Chap. 20

The same method can be used to find the full width at (1/m)Cmax . Shown in Fig. 20.18 are the FW.1M
(m = 10) and FW.02M (m = 50). These metrics are used to quantify the asymmetry of the full energy peak
with a skewness factor defined as 
FW(1/m)M ln 2
SR (m) = . (20.111)
FWHM ln m
For a symmetric Gaussian peak SR (m) = 1 for all m but for asymmetric peaks the skewness factors are greater
than unity. That full-energy peaks in a HPGe detector are asymmetric arises from the longer collection times
for charges created in low electric field regions of the detector compared to that for charges created in normal
regions. This longer collection time produces some signal attenuation when passing through an amplifier’s
linear pulse shaping network.6 Also Compton scattering decreases the signal in some pulses. The overall
result is an increase in the FW(1/m)M compared to the FWHM.

Example 20.5: Determine the corrected peak channel and counts for the peak shown in Fig. 20.18. The
peak is located between channels nL = 3351 and nR = 3374 and the observed three highest gross counts
are: GP = 10, 000 at channel 3365 and GE = 8910 and GF = 8748.

Solution:
First find the background corrections. From Eq. (20.103)

BL − BL 38 − 25.6
B(n) = BL − (n − nR ) = 38 − (n − 3351) = 38 − (n − 3351)(0.5391),
nR − nL 3374 − 3351
from which BE = 30.99, BP = 30.45, and BF = 29.91. Then N (n) = G(n) − B(n) so that

NE = 8879.01 NP = 9969.55 NF = 8718.09.

From Eq. (20.105) the continuous channel for the maximum counts is

(NE − NF )/2 80.46


ñmax = np + = 3365 + = 3364.96.
NE + NF − 2NP −2342
Finally from Eq. (20.106) the true maximum number of counts is

(NE − NF )2 (−160.92)2
Nmax = NP − = 9969.55 − = 9980.61.
8(NE + NF − 2NP ) −2342.00

In this case the peak correction is very small because NE is very close to NF . In fact if NE = NF there
would be zero correction to NP . The largest correction would occur when NP = NE or NP = NF .

Peak-to-Compton Ratio
Another metric specified for HPGe radiation spectrometers is the peak-to-Compton ratio (PCR). As de-
scribed in the ANSI/IEEE standard 325-1996, the measurement of the PCR is performed with the 1332.5
keV gamma-ray energy from 60 Co. The PCR is defined as

Cmax
PCR = , (20.112)
N

6 Gated-integrating pulse processing is less prone to this attenuation.


Sec. 20.5. Radiation Spectroscopy Measurements 1077

Figure 20.19. The peak-to-Compton ratio (PCR) is calculated by dividing


Cmax by N . In this example for a 20% ηrel HPGe coaxial detector the measured
PCR is 31.3. Courtesy of Nathaniel Edwards, KSU.

where Cmax = CP is the number of counts in the peak channel for the 1332.5-keV gamma ray and N is
the average number of counts per channel between the channels represented by 1040 keV and 1096 keV.
The energy range between 1040 keV and 1096 keV appears in the Compton gap of the 1173.2-keV gamma
ray of 60 Co; therefore, is almost entirely associated with the Compton continuum of the 1332.5-keV peak
(see Fig. 20.19). The environmental background B should be subtracted from the measurements before
calculating the PCR. The PCR metric is analogous to a sort of signal-to-noise ratio because the PCR is a
measure of the spectrometer’s ability to discern lower energy and lower count rate gamma-ray peaks in the
presence of higher energy gamma-rays and their corresponding spectral features.
As the energy resolution of a HPGe detector improves, the number of counts in the 1332.5-keV peak
channel increases. Also, as the size of the HPGe detector increases, so do counts in the 1332.5-keV peak
channel because fewer scattered gamma rays can escape the detector. Hence, improved energy resolution
and improved efficiency both tend to increase the PCR. PCR values can range from 30:1 for smaller HPGe
detectors up to over 90:1 for relatively large detectors [Gilmore 2008].
It is notable that prior versions of the IEEE ANSI standard 325 also included a PCR for 137 Cs in which
the maximum counts for the peak channel at 661.7 keV is divided by the average counts per channel in those
channels between 358 keV to 382 keV. Although the 137 Cs based PCR is generally not used to characterize
HPGe detectors, it still has utility as a benchmark for comparing PCR values for much smaller semiconductor
spectrometers, such as those with CdZnTe or HgI2 detectors whose peak efficiency at 1332.5 keV can be
small compared to that of a HPGe detector. However, this particular definition does not appear in the most
recent version ANSI 325-1996.

Peak-to-Valley Ratio
Another, less official, metric is the peak-to-valley ratio (PVR), which is measured with a 137 Cs source. This
metric is defined as the number of counts in the peak channel divided by the number of counts in the middle
of the Compton gap at 569 keV. This metric is seldom used for HPGe detectors; rather, it is more often
used for compound semiconductor detectors and (rarely) used for experimental scintillation detectors. This
1078 Radiation Measurements and Spectroscopy Chap. 20

metric provides a measure of the detector efficiency, energy resolution, and for semiconductors, a measure
of the charge carrier trapping effects.
Peak-to-Total Ratio
The peak-to-total ratio (PTR) is the ratio of the total counts in a full energy peak to the number of counts
in the entire spectrum. The metric is useful with monoenergetic gamma-ray sources, such as 137 Cs and
54
Mn, but is not well defined or interpreted for polyenergetic gamma-ray sources. The peak-to-total ratio is
proportional to the intrinsic full energy peak efficiency peak because
 
peak counts
peak = I = I PTR, (20.113)
total counts
where I is the total intrinsic counting efficiency. By carefully selecting monoenergetic gamma-ray sources,
the detector intrinsic peak efficiency can be calibrating over a broad energy range [Heath et al. 1967]. Unfor-
tunately, there are a limited few practical monoenergetic gamma-ray sources to conduct such a measurement.
Another method to accomplish this same task is to use two detectors in coincidence, with the detector
under investigation receiving the scattered gamma ray. The method entails capturing a Compton scattered
gamma ray that escapes from a high energy resolution primary (first) detector. The residual energy deposited
in the second detector is determined by subtracting the energy deposited in the first detector from the known
emission energy. Collimation and pulse height discrimination can be used to select and allow only scattered
gamma rays of a specific energy, thereby producing a pulse height spectrum, at the energy under investigation,
from the second detector.

20.5.3 Detection and Spectroscopy with Scintillators


The properties and advantages of scintillators are described in Chapter 13. Added here are some specific
details on spectroscopic measurements and performance pertinent to scintillators. The quality metrics used
to assess the photon spectroscopy performance of scintillation detectors include the energy resolution, the
peak-to-total ratio (PTR), the intrinsic peak efficiency (I ), and the escape peak efficiency (es ) [Heath 1964].
Usually performance comparisons between different scintillation materials and detectors are conducted with
661.7-keV gamma rays from 137 Cs.
Recall from Chapter 4 that the photon interactions important to gamma-ray counting and spectroscopy
are photoelectric, Compton scattering, and with sufficient energy, pair production. The combined intrinsic
gamma-ray interaction efficiencies that any one of these interactions occurs are plotted in Chapter 13,
Figs. 13.13, 13.14, 13.15, 13.17, 13.19, and 13.20 as a function of photon energy for several scintillation
materials. An often used method to predict gamma-ray detection performance is to couple the solid angle
calculations (from Chapter 7) with the interaction efficiencies, a method repeated in many textbooks on
radiation detection and measurements. These complicated calculations often include parallax effects as well.
Although useful in determining the probability of an interaction occurring, and perhaps assisting with the
overall determination of counting efficiency, these methods do not yield information on the energy deposited
nor the expected spectral features. Monte Carlo techniques can instead be used to calculate the photon
energy deposition and the resulting spectroscopic features and respective intensities with increased accuracy
above that of previously used graphical and empirical methods.
Detector Geometries
Commercial scintillators can be acquired in a variety of geometries and configurations, ranging from indi-
vidual crystals to integrated packages with light collection device, voltage divider, and preamplifier. Many
of the alkali metal and halogen based scintillators, such as NaI:Tl, LiI:Eu, CLYC:Ce, SrI2 :Eu, LaBr3 :Ce and
CeBr3 are highly hygroscopic. Hence, commercial material is usually obtained already packed in a hermeti-
cally sealed reflective cannister that can be attached to a light collection device of choice. Large devices are
Sec. 20.5. Radiation Spectroscopy Measurements 1079

usually configured as right circular cylinders, while smaller devices can be obtained as either cylinders or
cuboids. The cylindrical shape is convenient for coupling to common circular PMTs, while the small cuboid
shapes are convenient for coupling to SiPMs. Proper selection of a scintillation crystal requires that the
response function of the chosen light collector match the scintillator emission spectrum (see Sec. 13.2.2 and
Fig. 13.3). Also, to avoid space charge distortion in a PMT, the response speed of the PMT should be fast
enough to follow the light emissions. This requirement is especially important for bright and fast scintillators
such as LaBr3 :Ce, LaCl3 :Ce, and CeBr3 . If a proper response speed is not selected, current crowding and
space charge buildup result in a non-linear output (see discussions in Sections 13.2.3, 14.1.7, and 14.1.8).
For high-energy gamma rays interacting in bright scintillators, similar problems occur with SiPMs in which
the probability of coincident light photons interact in the SPADs (see Sec. 14.2.4).
Although commercial vendors may provide just the scintillator for custom work, it is far more common
that scintillators are obtained already coupled to the light collection device. Hence, the total package is
usually already optimized with the proper coupling compound, shielding, glass envelope, spectral response
and electronic output. Commercial vendors quote the optimum operating conditions, including recommended
voltage and count rate limitations. Specification sheets usually list the performance metrics mentioned above.
NaI:Tl, discovered by Hofstadter in 1948, remains the most commonly used scintillator for general gamma-
radiation spectroscopy applications. The reasons for this widespread usage include its relatively low cost,
the fact that large crystals can be produced, and the gamma-ray interaction efficiency is adequately large
(because of the iodine component). The general application of NaI:Tl to radiation spectroscopy is reviewed
by Smith and Kearfott [2018]. It is the 3 in × 3 in right circular cylinder of NaI:Tl that is quoted most
often in performance comparisons to other spectrometers (scintillators and semiconductors), although a wide
variety of NaI:TL sizes are available. Some of these alternative shapes include large plates for Anger cameras,
pixelated arrays, well detectors, long bars, cuboids, spheroids, annuli for Compton suppression, and curved
crystals.

Right Circular Cylinder Detectors The right circular cylinder is the most common geometry for scintil-
lation detectors, mainly because the flat circular face conveniently couples well to cylindrical PMTs. The
nomenclature for detector size is the diameter × length. For example, a 2 in × 3 in size describes a 2 in
diameter by 3 in long detector. Common commercial sizes are 1 in × 1 in, 2 in × 2 in, 3 in × 3 in, and
5 in × 5 in, although some companies can provide custom sizes for an added charge. The common use of
m × n dimensions where m = n is with purpose, mainly, the light is distributed more uniformly over the
photocathode of the PMT. This uniformity produces the best energy resolution, and deviations from this
ratio have a poorer resolution. Solid angle corrections for cylindrical geometry are described in Sec. 7.4,
and spectroscopic performance for NaI:Tl detectors are well documented by several authors [see for example
Heath 1964; Crouthamel 1970].

Well and Annular Detectors Some scintillation detectors, called well detectors, are available as a cylinder
with a blind hole or well drilled in them. These detectors are designed to perform, nearly, as a 4π detector,
where the sample under investigation is placed at the bottom of the well. The probability that an isotropically
emitted gamma ray enters the crystal is

d
P ≈ .5 1 + √ , (20.114)
d + a2
2

where d is the well depth and a is the well radius. However, because of different attenuation lengths through
the crystal, especially at corners, the probability of interacting in the detector changes with the gamma-ray
trajectory. Further, as explained previously, the interaction efficiency (actually the interaction probability)
does not describe the efficiency of total energy deposition. Hence, well detectors may increase the total
1080 Radiation Measurements and Spectroscopy Chap. 20

counting efficiency, but the intrinsic peak efficiency may suffer from added Compton losses at the extended
boundary, especially as the gamma-ray energy increases.
If, instead, a smaller detector (small scintillator or semiconductor) is located inside the well, the well de-
tector can be used as a Compton suppression coincidence detector (reviewed later in this chapter). Annular
detectors are also used for Compton suppression, where the scintillation detector is a larger ring that sur-
rounds a relatively large detector such as an HPGe detector. The annular detector may be a single annulus,
or may be composed of annular segments that form the ring.
Position Sensitive Detectors A long bar of scintillator with a light detector at each end can be used
as a position sensitive gamma-ray detector. Light radiates from the ionizing path of the particle, be it a
photoelectron, Compton electron, or charges produced by pair production. This light generally decreases
exponentially in magnitude as it propagates through the crystal. Consider the configuration of Fig. 20.20
where an ionizing event produces light originating at position x along a scintillator bar of length L. For
L isotropic generation of scintillation photons and with the same
x notation used in Sec. 13.2.2, PMT A produces an induced charge
signal

QA = fA qe M Ne En Fn Cnp UA e−αx  KA En e−αx , (20.115)


PMT A PMT B
L/2 L/2

where En is the ionizing particle energy, qe is the unit charge,


Fn is the fraction of energy deposited in the detector, Cnp is the
Figure 20.20. Depiction of a scintillator bar de-
tector used for position sensitive measurements.
average light conversion efficiency (light yield), Ne is the charge
released from the photocathode, M is the PMT gain, fA is the fraction of photons that propagate generally
in the direction of PMT A, and UA accounts for nonuniformities in light collection from geometrical effects,
and α is the attenuation coefficient. The induced charge from PMT B is, therefore,

QB = fB qe M Ne En Fn Cnp UB e−α(L−x) ≡ KB En e−α(L−x) (20.116)

The ratio of the PMT signals is

SA QA KA En e−αx
≡ = = C1 e−2αx+L (20.117)
SB QB KB En e−α(L−x)

By adjusting the gain M of either PMT, the value of KA can be made equal to KB , hence C1 becomes equal
to unity. Carter et al. [1982] define x = x − (L/2) so that Eq. (20.117) yields

SA 
= e−2αx . (20.118)
SB

Hence, taking the natural log of Eq. (20.118) yields a relationship for the interaction position
 
1 SB
x = ln (20.119)
2α SA

The corresponding standard error is


*  
+1/2
eαL/4 eαx e−αx
σx = √ + . (20.120)
2α En KA KB
Sec. 20.5. Radiation Spectroscopy Measurements 1081

If KA = KB = K, then Eq. (20.120) becomes


*  
+1/2
eαL/4 eαx + e−αx
σx = . (20.121)
2α En K

Substituting Eq. (20.119) into Eq. (20.118) yields the interaction position
 
1 SB L
x= ln + . (20.122)
2α SA 2

and
 1/2
eαL/4 eα(x−L/2) + e−α(x−L/2)
σx = . (20.123)
2α En K
Finally, to find the initial gamma-ray energy En multiply Eqs. (20.115) and (20.116) to obtain

QA QB = KA KB En2 e−αL = K 2 En2 e−αL . (20.124)

Then solving this result for En gives



QA QB αL/2 
En = 2
e = C2 SA SB eαL/2 , (20.125)
K
where the constant C2 accounts for signal conversion from the induced charges. From the results of
Eqs. (20.119) and (20.124), it is shown that the linear position and energy of an event can be measured
with the relatively simple arrangement of Fig. 20.20. For a NaI:Tl bar with dimensions of 5 cm × 5 cm ×
50 cm long, Carter et al. [1982] report a position resolution for 661.7-keV gamma rays of 10 mm ± 10% at
the center and approximately 12 mm ± 12% at the ends.
Pixelated scintillation detectors are banks of scintillator rectangular prisms fastened together with thin
Lambertian layers called “separators”. These separators range in thickness from 0.5 mm down to 0.04 mm
depending on type, and differ in relative reflectivity, with powders of TiO2 and MgO2 being amongst the
highest in both reflectivity and thickness. The light emissions from these segmented crystals are isolated;
hence, by attaching the array to a position sensitive PMT or SiPM, the xy spatial location of an event can
be determined [Saint Gobain, 2019b]. To increase light collection, a Lambertian reflector is applied over the
array surface opposing the light detector. There are several types of commercial arrays of prismatic crystals,
including CsI:Tl, BGO, LYSO, and CdWO4 . The prism sizes are constrained by material limitations, but
are generally on the order of 0.3 to 0.8 mm long with side dimensions on the order of 0.3 to 1 mm.
These pixelated arrays are designed for radiation imaging such as computed tomography or other radi-
ation imaging techniques. In principle, the same method described for linear position sensing can be used
to determine the z spatial component, making the device a volumetric position sensitive device. However,
because of the small prism sizes, Compton escapes into adjacent crystals are relatively probable. To ame-
liorate this effect, the output can be summed to assist with energy identification and to increase the overall
intrinsic peak efficiency. The energy resolution, however, is decreased because of the variation in energy lost
in the insensitive separator layers.
An alternative approach has been to grow columnar structures of CsI:Tl, each crystal column being on
the order of a micron in diameter and typically are less than 600 microns long, but apparently special units
up to 1.5 mm can be obtained [Bugby et al. 2016]. The columns perform as optical light guides that direct
light to the column ends. Due to the small thickness, this imaging scintillator is best used for x-ray energies.
1082 Radiation Measurements and Spectroscopy Chap. 20

The columnar crystal structure is attached to a photon imaging device, which delivers the xy spatial position.
A reflective coating can be used to help collect light that transports, initially, in the opposite direction of
the position sensitive light detector. Plates on the order of 440 mm × 440 mm are commercially available
[Hamamatsu 2016].
Ruggedized Units Many scintillators are extremely fragile, and mishandling can lead to catastrophic frac-
tures induced by mechanical shock that can permanently damage the crystal. However, there are certain
ruggedized designs that resist this problem. For instance, polycrystalline NaI:Tl compressed under high
temperature conditions can eliminate differences in the index of refraction at the grain boundaries. Hence,
light transports through the device in the same fashion as a single crystal. However, fractures induced in
a single crystal grain are confined to that grain and do not propagate across the device. These ruggedized
units have been developed for the oil well logging industry to meet the stringent demands on instrumentation
for in situ measurements, including heat resistant seals and electronics.7
Low Background and Low Energy Detectors For low-level radiation measurements, special units composed
of scintillators and supporting electronics with relatively low background levels are commercially available.
Much of the low-level background contamination comes directly from 40 K in the PMT glass envelope. The
problem is greatly mitigated by using purified quartz as the PMT envelope, or at least as the main coupling
window. Also, the metal housing is made with purified low background stainless steel or copper. The
scintillator itself may be contaminated with a background source.8 Hence, careful selection of purified
scintillators without radioactive constituents is preferred.
Low energy gamma- and x-ray applications require special crystal thicknesses that are adequately efficient
only at low energies, with higher energy photons either passing through without interaction or depositing
only a fraction of their energy. Also, the thickness and material of the entrance window must be altered to
allow the efficient passage of low-energy photons. Common choices are beryllium and aluminum, with the
former having an energy range between 3 to 100 keV with the latter having an energy range between 10
to 200 keV. Note that NaI:Tl is often selected for low-energy low-background scintillation detectors. The
relative light yield at low energy increases (see Fig. 13.4), improving the crystal performance at energies
below approximately 100 keV. The phoswich detector, presented later in this chapter, is another detector
configuration specifically designed for low-energy gamma-ray measurements. Anti-coincidence methods can
reduce the number of Compton scattering events, thereby enhancing the appearance of the gamma-ray full
energy peaks.
Energy Resolution
The energy resolution describes the spectroscopic performance of a scintillation. For scintillators this par-
ticular metric is traditionally reported as a percent FWHM of the peak energy
ΔE
FWHM% = 100 , (20.126)

where ΔE is the FWHM in units of energy. It is common to quote energy resolution for scintillation detectors
at 661.7 keV for gamma rays from 137 Cs. Typical energy resolution ranges from approximately 3% FWHM
at 661.7 keV for some of the high-performance scintillators (LaBr3 :Ce, CeBr3 , CLLB:Ce), while traditional
scintillators such as NaI:Tl have energy resolution on the order of 7% FWHM at 661.7 keV, or approximately
47 keV FWHM. The energy resolution affects the ability to distinguish neighboring gamma-ray energies.
Hence, gamma-ray peaks closer than 47 keV apart significantly overlap.

7 For instance, the Polyscin R NaI:Tl detector developed by Saint Gobain Crystals is designed to withstand shock and vibration
for temperatures between 55◦ C and 205◦ C.
8 Such as 138 La and 227 Ac in LaCl and LaBr .
3 3
Sec. 20.5. Radiation Spectroscopy Measurements 1083

The energy resolution of a scintillator is a function of multiple processes, which include the light conversion
efficiency, the relative light yield linearity, light collection efficiency, and conversion gain and linearity of the
light detector. Given an average photon yield per energy deposited, the percent energy resolution can be
generally described by Eq. 13.36, rewritten here as

1.1
FWHM% ≈ 235.5 , (20.127)
N
where N is the average number of photons released for the energy under investigation. Assume that the
value of N is a linear function of the gamma-ray energy, where

N = Cnp Eγ (20.128)

and Cnp is average light yield per MeV. Then


<
1.1
R = FWHM% ≈ 235.5 = C1 Eγ−1/2 , (20.129)
Cnp Eγ

where C1 is a constant. Beattie and Bryne [1972] show that Eq. (20.129) can be described as a linear equation
1
ln(R) = ln(C1 ) − ln(Eγ ) (20.130)
2
as plotted in Fig. 20.21 for several gamma ray energies recorded with a NaI:Tl detector.
As a general rule, bright scintillators are sought because the increased photon yield should increase the
value of N , and from Eq. (20.127) should also improve the energy resolution. However recall from Sec. 13.2.2
that linearity of the relative light yield also has a significant effect. For example, from Table 13.1, NaI:Tl
has a light yield of 43000/MeV, while LaBr3 :Ce has a light yield of 63000/MeV. Hence, it would be expected
that LaBr3 :Ce would have approximately 1.21 times improved energy resolution over similar sized NaI:Tl
detectors. However, energy resolution also depends on spectral matching to the light collection device and
the linearity of the relative light yield. From Fig. 13.3, NaI:Tl matches better to common PMTs than
does LaBr3 :Ce, yet comparing Figs. 13.4 and 13.5, LaBr3 :Ce has a superior linear response at low energies.
Consequently, the energy resolution of LaBr3 :Ce is far superior to that of NaI:Tl than might be surmised
from Eq. (20.127), as can be observed by the spectral comparisons in Fig. 20.22. Overall, energy resolution
generally improves with scintillator brightness and relative light yield linearity.
Peak-to-Total Ratio
Shown in Fig. 20.23 are PTR values for several NaI:Tl detector sizes, source distances, and gamma-ray
energies. Intuitively, the PTR decreases with increasing gamma-ray energy and increases with detector size
[Leutz et al. 1966], being best for a collimated gamma-ray beam striking the detector. From Fig. 20.23, it
is also notable that the PTR is nearly the same for similar detector sizes regardless of source distance and
collimation. The PTR increases, generally, with the effective Z and mass density of the scintillation material.
Shown in Fig. 20.24 are calculated PTR values as a function of energy for several different commercial
scintillator materials. Clearly the materials with higher Z components have the highest peak-to-total ratios,
while the lightest material shown (CaF2 ) has the lowest.
Intrinsic peak efficiency
Because the PTR is the ratio of peak /I (see Eq. (20.113)), it is also noted that the full energy peak efficiency
increases with PTR. When counting efficiency is most important, for instance in medical imaging applica-
tions, then often materials with high Z, and ultimately a high PTR, are attractive choices. Materials that
1084 Radiation Measurements and Spectroscopy Chap. 20

Figure 20.21. Experimental values of energy resolution for a NaI:Tl detector


compared to a least squares fit. The gamma ray energies have been converted
into units of electron rest mass (511 keV). Data from Beattie and Byrne [1972].


,-.&'/0
,-.()*/0
 ,-.+& )" /0
!"# $%

 &'
+& )"

 ()*
 






         
   
Figure 20.22. Comparison of normalized spectral performance for a 2×2 NaI:Tl
detector, a 2×2 LaBr3 :Ce detector, and a BGO detector of similar size for 662
keV gamma rays from 137 Cs. BGO data from Vincke et al. [2002] and LaBr3 :Ce
data from Quarati et al. [2007]. NaI:Tl data courtesy of Taylor Ochs, KSU.
Sec. 20.5. Radiation Spectroscopy Measurements 1085

Figure 20.23. Peak-to-total ratios for NaI:Tl detector of different sizes for different gamma ray energies, showing from left to
right the results of a point source located 50 cm from the face center, 10 cm from the face center, and a collimated beam 0.7
cm diameter. Data from Leutz et al. [1966].

Figure 20.24. Monte Carlo calculated comparisons of peak-to-total ratios for


a collimated beam of gamma rays for several commercial scintillators. The
data is for 3 in × 3 in right circular cylinders. Data from Saint Gobain [2016].
1086 Radiation Measurements and Spectroscopy Chap. 20

generally have high Z elements typically have better intrinsic peak efficiencies than those composed of low
Z materials. For instance, the plot in Fig. 20.24 indicates that BGO should have a relatively higher intrinsic
peak efficiency than LaBr3 :Ce, which should have higher peak efficiency than NaI:Tl. This correlation can
be observed from the normalized spectra shown in Fig. 20.22, where clearly BGO has the highest peak value
while NaI:Tl has the lowest peak value of the three scintillators in the example. Note also that the Compton
continuum has relatively more counts for the NaI:Tl detector than either the BGO or LaBr3 :Ce detector, an
indication that the NaI:Tl detector has more scattered photon losses. Overall, the plots like Fig. 20.24 can
also yield some indication of the expected intrinsic peak efficiencies.
Summary
The primary disadvantages of scintillator spectrometers are (1) that a photon detector such as a PMT
must be incorporated into the device and (2) that the energy resolution is inferior to that of a semiconductor
spectrometer. Historically, scintillation crystals were coupled to PMTs so that the spectrometers were fragile
and bulky. A special μ-metal is also needed to shield the PMT from magnetic fields. Modest success was
realized with the coupling of scintillators to semiconductor photodiodes, yet the energy resolution was inferior
to that obtainable with a PMT. The introduction of the silicon photomultiplier (SiPM) has greatly reduced
the problem of fragility of PMTs and their bulkiness while nearly preserving the energy resolution achieved
with PMTs. Scintillator spectrometers of many varieties coupled to SiPMs are now commercially available
as rugged and compact devices unaffected by magnetic fields and provide nearly the same energy resolution
as their PMT-coupled counterparts. Regardless of these new benefits, the spectroscopic performance of
scintillators remains inferior to semiconductor spectrometers, especially to that of high-purity Ge and Si
spectrometers (see Fig. 20.25).

20.5.4 Spectroscopy with Semiconductors


The physics and performance of semiconductor detectors are described in Chapters 15 and 16, including
sections on device designs, efficiencies, and energy resolution. A few more details are offered here that are
pertinent to radiation spectroscopy with semiconductor detectors. Otherwise, the general discussions on
spectroscopy found elsewhere in this chapter also apply to semiconductor detectors.
IEEE Standard for HPGe Peak Efficiency The detection efficiency of a HPGe detector is defined in ANSI
325-1996, and is actually an absolute efficiency under a specific geometry. A calibrated point 60 Co source is
placed exactly 25 cm from the center of the cryogenic end cap face of a HPGe detector. The source activity
is calculated and the total number of counts appearing in the 1332.5 keV full energy peak is divided by the
total number of 1332.5-keV gamma rays emitted by the source during the measurement. The ANSI 325-1996
document suggests that a pulser set at an energy channel 5% higher than 1332.5 keV (≈ 1400 keV) can be
used for timing calibration.9
A background measurement is conducted without the 60 Co source present. After subtracting the back-
ground spectrum (as described earlier in Sec. 20.5.2), the absolute efficiency of the HPGe detector is then
quoted as
Ap
ηa = 100 %, (20.131)
Ns
where Ap is the integrated number of counts (area of) in the 1332.5-keV background-corrected full energy
peak and Ns is the total number of 1332.5-keV gamma rays emitted by the 60 Co source during the measure-
ment live time. It is assumed any source or air absorption is negligible.

9 The concrete of radiation counting laboratories may be contaminated with 40 K, which emits a 1460.8 keV gamma ray. Although
the energy 1400 keV falls in the Compton gap of the 40 K spectrum, the possible interference from 40 K can be eliminated
altogether by setting the pulser at 15% above 1332.5 keV (1530 keV).
Sec. 20.5. Radiation Spectroscopy Measurements 1087

Figure 20.25. Comparison gamma-ray spectra of 60 Co taken with a NaI:Tl


detector and an HPGe detector.
Traditionally, the efficiency of a HPGe detector is quoted as a relative comparison to the expected
efficiency of a 3 in × 3 in (or 7.62 cm × 7.62 cm) NaI:Tl detector.10 Such an efficiency is referred to as the
relative efficiency. The expected number of counts per unit activity in the 1332.5-keV full energy peak of
such a NaI:Tl detector, when set back 25 cm from the source, is well established as 0.0012 cps per Bq. The
measurement is conducted, as before, with a calibrated 60 Co source placed exactly 25 cm from the center of
the cryogenic end cap face of a HPGe detector. After first subtracting the background spectrum, the relative
efficiency is found as
Ap
ηrel = 100 %, (20.132)
0.0012 × A60 Co
where A60 Co is the activity of the source at the time of the measurement. It is this relative efficiency
that is usually quoted for coaxial HPGe detectors. However, because other (non-coaxial) HPGe detector
configurations may not be efficient at 1332.5 keV, the relative efficiency is usually not used for non-coaxial
designs. Usually the manufacturer makes clear the standard being used to report detector efficiency.
Reporting Energy Resolution The energy resolution dependence for semiconductors was derived in
Sec. 16.3.2, repeated here for convenience,
 
FWHMenergy = 2 2 ln(2)wF En ≈ 2.355 wF En , (16.24)

where w is the average ionization energy, En is the radiation particle energy, and F is the Fano factor. For
semiconductor detectors the energy resolution is traditionally reported in units of keV for both gamma-ray
and charged particle detectors. The reason for this standard is that the energy resolution is generally below
1% FWHM for high-performance semiconductors, and reporting the FWHM in terms of percent generally is
less descriptive than reporting the actual energy. Regardless, there has been a departure from this historic

10 Thishistoric standard dates from the early introduction of semiconductor detectors, when it was common to directly compare
efficiency to what had become the standard for gamma-ray spectroscopy, the 3 × 3 NaI:Tl detector.
1088 Radiation Measurements and Spectroscopy Chap. 20

standard for some of the lower resolution compound semiconductors, and often the energy resolution FWHM
is reported in terms of percent for compound semiconductors.
HPGe detector energy resolution has historically been measured at 1332.5 keV (one of the gamma rays
emitted by 60 Co) and is also the IEEE standard. However, because compound semiconductors are typically
smaller and have less efficiency at 1332.5 keV, the energy resolution of these devices is commonly reported
at 661.7 keV (a gamma ray emitted by 137 Cs). Si(Li) detectors are relatively inefficient at energies below
60 keV, and are generally reserved for use at lower energies. Typical gamma-ray energy resolution is on the
order of approximately 2 keV FWHM at 1332.5 keV for some of the high-performance HPGe detectors, and
around 200 eV FWHM at 5.9 keV for Si(Li) x-ray detectors. The more mature compound semiconductors
(CdTe, HgI2 , CdZnTe) typically have between 6 to 20 keV FWHM at 661.7 keV.

20.6 Factors Affecting Energy Resolution


The energy resolution achievable from a spectrometer is largely determined by the average energy required
to produce a fundamental signal carrier, statistical fluctuations in signal carrier production, non-linearity in
signal carrier production, and electronic noise. Energy resolution is also compromised by non-linear light
yield in scintillators. In semiconductors, charge carrier recombination and trapping produces non-linear
charge collection and affects the resolution. Electronic noise also adds to the variance in the pulse height
distribution. Common factors that affect the energy resolution of radiation spectrometers are discussed
below, with the emphasis on scintillation and semiconductor spectrometers. Also discussed are the primary
sources of electronic noise, which also affects the resolution.
Variation in Charge Collection
The production of information carriers in a spectrometer is usually modeled as a Gaussian process. For in-
stance, the average number N eh of electron-hole pairs produced by a gamma-ray in an HPGE semiconductor
detector is the gamma-ray energy absorbed Eγ divided by the average ionization energy w. In Sec. 16.4.2,
a Fano factor F was used to correct for differences from Gaussian predications, i.e., σ 2 (N eh ) = F N eh . For
semiconductors, the Fano factor is usually on the order of 0.1, but varies between materials as can be seen
from Table 16.2. Hence, the energy resolution in terms of energy is defined by
 
FWHMenergy = 2 2 ln(2)σeh (f )Eγ = 2.355 wF Eγ . (20.133)

It is apparent the FWHM increases as the square root of the gamma-ray energy. Traditionally, the energy
resolution of a semiconductor spectrometer is reported in units of keV. However, for some applications, the
percent energy resolution is of interest, namely
<
wF
FWHM% = 235.5 %. (20.134)

Equations (20.133) and (20.134) are relatively good predictors for well-behaved semiconductors that do not
suffer from severe recombination or trapping. However, large losses from charge carrier trapping cause the
full energy peak to distort, as shown by examples in Sec. 15.5.1, with the development of a low-energy tail
on the low-energy side of the full energy peak. If trapping is severe, the tail can cause such a large distortion
that a full energy peak is difficult or impossible to discern.
Scintillator Non-linearities
Another source of variance in the number of signal carriers is due to a non-linear light yield response to
deposited gamma-ray energy in many scintillators as shown in Figs. 13.4 and 13.5. Although the average
photon yield is often estimated by the product Eγ and the average light yield per unit energy (photons/MeV),
Sec. 20.6. Factors Affecting Energy Resolution 1089

such an estimate is based on a linear response. For many scintillators, the non-linearity in light yield can be
severe for gamma-ray energy deposition below 500 keV. Hence, the manner by which a photon interacts in
the scintillator affects the total light yield. For example, a 1.332-MeV gamma ray completely absorbed by the
photoelectric effect produces less light in NaI:Tl than if the photon scattered twice, depositing approximately
400 keV for each scatter before finally being absorbed by the photoelectric effect. Even though the same
amount of energy is absorbed in both cases, the amount of light produced is different and, thus, increases
the variance in the output signal. Consequently, scintillators with a linear response, but perhaps lower light
yields, can still perform well. An example is YAP:Ce, which is a linear scintillator with about 40% of the
light yield produced by NaI:Tl. Although not as bright, the energy resolution of YAP:Ce has been reported
at 4.4% FWHM at 661.7 keV, much lower than NaI:Tl (typically greater than 6% FWHM at 661.7 keV).
The output from the light collection device, a PMT for example, also contributes to the total variance as
quantified by Eq. (13.30). Traditionally, the energy resolution at FWHM is reported in terms of percent for
scintillators.

Electronic Noise
Electronic noise arises from fluctuations in the speed and number of electrons and is present in both pulse
mode and current mode detector systems. The fluctuations may be from thermal effects, leakage currents, or
generation-recombination effects and may originate in the actual detectors and/or in the system electronics.
Regardless of the source, electronic noise determines the minimum FWHM energy resolution that is possible
for a given detector and its associated electronics. Noise from current fluctuations is commonly named
parallel noise, while noise from voltage fluctuations is often called series noise. Thermionic leakage current
from a reverse biased diode produces shot noise, while resistors produce Johnson noise. The appearance of
so-called periodic 1/f noise, where f is the noise frequency, is a consequence of non-random emissions, such
as carrier generation and recombination, or trapping and detrapping, in the detector or system electronics.
The goal in designing a detector system is to reduce the electronic noise as much as possible, so as to improve
the signal-to-noise ratio η (SNR), defined as the ratio of the detector mean signal pulse voltage Vavg to the
square root of the mean-square noise voltage (the variance in the noise Vn2 ), i.e.,

Vavg
η= . (20.135)
Vn2

As discussed in Chapter 22, if the noise is modeled as a Gaussian distribution, then the contribution to the
detector and system energy resolution can be approximated by

VFWHMnoise Vn
= 2.355 . (20.136)
Vavg Vavg

Ultimately, this contribution to the variance must be added, by error propagation, to the other resolution
limiting variances to predict the overall detector resolution

FWHM = (FWHMnoise )2 + (FWHMtrap )2
1/2
+ (FWHMeh )2 + (FWHMnon−linear )2 + . . . . (20.137)

The electronic noise component FWHMnoise can be measured by inserting an electronic pulser into the
system. The pulser delivers a constant voltage pulse into the system, usually through the preamplifier, and
the FWHM of the pulse can be directly measured. The square of this measurement can be subtracted from
the square of Eq. (20.137) to determine the limiting resolution of the actual detector.
1090 Radiation Measurements and Spectroscopy Chap. 20

20.7 Experimental Design


Proper experimental design can make the difference between an accurate and a questionable measurement.
Previously in Chapter 6 there was some discussion about the minimal detectable activity (MDA) and the
critical detection limit (CDL). These measurements are used when the radiation activity of interest is similar
to that of the background. There are also situations in which discernment between similar energies is impor-
tant, an issue partly covered in Sec. 20.4.8 of this chapter. Rather than just start by making measurements,
an experimental outcome can be generally much improved by designing a procedure or protocol for the
experiment before the taking measurements. Some experimental design considerations are described here.

20.7.1 Optimization of Measurement Time


Sometimes the time allocated tA to an experimenter to use a particular system that is in high demand is
limited, such as with a low-level deep-underground counting facility. In such cases it is important to optimize
the counting times for the background and the source or foreground measurements so as to minimize the
uncertainty in the background corrected source measurements.
A Single Source Measurement
In this case the allowed time tA must be divided between the time tG for the foreground or source measure-
ment and the time tB for the background measurement. Typically, the background count rate b is subtracted
from the count rate g observed for the source measurement to determine the net counting rate n, and the
two independent measurements are used to calculate the experimental error. Minimizing this error can be
achieved by optimizing the foreground measurement time tG and the background measurement time tB ,
subject to the constraint tA = tG + tB . The radiation counting rate g, which represents contributions from
both the radioactive or foreground source and the background, is

G
g= , (20.138)
tG
where G is the total number of counts recorded during time tG . The background counting rate is

B
b= , (20.139)
tB
where B is the total number of background counts recorded during time tB . The net counting rate is

G B
n=g−b= − , (20.140)
tG tB
The estimated net counting error, as derived in Sec. 6.9.2, is
1/2
G B
σ(n) = + 2 (20.141)
t2G tB
or
g b
σ 2 (n) = + . (20.142)
tG tB
To optimize this result with the total allowed time fixed at tA = tG + tB Eq. (20.142) is differentiated as
" #
dσ 2 (n) d g b g b
= + =− 2 + (20.143)
dtG dtG tG tB tG (tA − tG )2
Sec. 20.7. Experimental Design 1091

and this result is set to zero to find tG /tB to produce the minimum σn2 . The result is

g b b
= = 2 (20.144)
2
tG (tA − tG )2 tB
or 
tG g
= . (20.145)
tB b
This result may seem counter-intuitive because it implies that the higher the source count rate is to the
background count rate, the smaller is the fraction of the available time that should be given to determine
b. But if g b, then the background has a very minor influence on the net count rate and hence need not
be determined very accurately. However, there is one obvious problem with this optimization procedure.
To use it, the experimenter must already have knowledge of the expected background count rate b and the
expected radiation response rate g. Such a priori knowledge must be obtained from past experience or initial
measurements of small duration.

20.7.2 Discernment Between Two Outcomes


Determination of the appropriate number of counts in a measurement is straightforward for a measurement
with little or no background and no overlapping energy peaks. However, for low-level counting and for iden-
tification of isotopes emitting gamma rays of almost equal energies, it is necessary to design the experiment
to discern the correct result among multiple possibilities.
Suppose there is a measurement background with rate b recorded by your detector and you have a sample
which yields a count rate g with a source. This result can be for any source that deposits sufficient energy
to provide a count in the measurement. Hence, g is the sum of the background count rate b and the source
count rate or net rate n. The problem is that the measurement of g includes both background and source
detector events. Typically, it is sufficient to simply subtract the background rate from g to obtain n, but
at times the rate of the measurements may be extremely low. Hence, some understanding of the minimum
number of total counts required is necessary.
If the background measurement time is tB and source measurement time is tG , how many counts must
be recorded to provide confidence in the measurement? For a Gaussian model, the average number of
background counts is 
B = btB ± btB , (20.146)
and the average number of recorded source counts is

G = gtG ± gtG . (20.147)

If gtG is relatively large compared to btB , then it is easy to distinguish between the two measurements.
However, if gtG is similar to btB , it is difficult to determine the actual source activity. This problem is
addressed in Sec. 6.10.1, in which the minimum detectable activity (MDA) and critical detection limit
(CDL) were examined and practical results were determined. Here the discernment between two possible
outcomes is considered.
Consider a situation in which identification of a collection of events is a function of a theoretical average.
The tallied events may be a collection of counts or a collection of pulse heights. If the outcome of two such
averages are similar, how does one identify the proper outcome? For instance, if two gamma-ray energies
from different isotopes are similar, how does one identify the proper isotope? Detectors with high energy
resolution reduce this uncertainty, a consequence of the Gaussian spread about the peak channel, but do not
totally eliminate the uncertainty. A similar situation exists in radiation counting where two predictions from
1092 Radiation Measurements and Spectroscopy Chap. 20

Figure 20.26. The situation in which two similar possible experimental out-
comes exist, either C1 = c1 t or C2 = c2 t.

different phenomena (e.g., counting rate or efficiency) may be similar. Hence, a measurement is conducted
that results in a collection of counts within a time period, the outcome of which can be easily misinterpreted.
Assume a count rate c1 for one outcome and a count rate of c2 for a second but similar outcome. The
total number of events is either c1 t or c2 t where t is the observation time. In either case, the expected
outcome has experimental uncertainty such that the number of events observed for ci t is

Ci = ri t ± ri t, i = 1, 2. (20.148)
What then is the probability of an incorrect conclusion? The situation is best understood with the help of
Fig. 20.26. If the outcome is identified as the average count rate c1 , what is the probability that it is actually
c2 , and if c2 is chosen, what is the probability that it is actually c1 ? The uncertainty in this situation can
be decreased by first deciding on an acceptable error kσ, and then conducting a measurement to ensure that
adequate counts are acquired. Note that the average count rate does not change for either situation, but the
uncertainty for either situation decreases as more counts are accumulated.
The probability distributions for C1 and C2 are assumed to be Gaussians, and a portion of the two
probability distributions overlap, represented by the shaded area in Fig. 20.26. If a condition is set that
the outcome is identified as C1 provided that the measured result is below C1 + k1 σ(C1 ), where k1 is the
number of standard deviations from the mean of C1 , then the shaded area β represents the probability
that the outcome is actually C2 . If instead the outcome is identified as C2 if the measured result is above
C1 + k1 σ(C1 ), then the shaded area α represents the probability that the outcome is actually C1 . The
difference between the averages of the two possible outcomes is represented by
ΔC = C2 − C1 = [k1 σ(C2 ) + k2 σ(C1 )], (20.149)
where k2 is the number of standard deviations from the mean of C2 . Because the two distributions are
relatively close, it can be assumed that at the crossover point k1  k2 so that
 
ΔC = C2 − C1  k(σ(C1 ) + σ(C2 )) = k( C1 + C2 ). (20.150)
Sec. 20.7. Experimental Design 1093

From this result  


C1 = C2 − k( C1 + C2 ). (20.151)
The measurement time can now be adjusted to increase the value of k by increasing the Ci , which are related
by
C2 − C1
k=√ √ . (20.152)
C1 + C2
The theoretical outcomes C1 and C2 are calculated from the measurement time t. For example, if k = 1.65,
then the shaded area α or β represents 5% of either Gaussian distribution and indicates the possibility of a
5% error for either outcome at the point C1 + kσC1 . To decrease this error to only 1%, then the calculated
outcomes must change such that k = 2.33, which can be accomplished by increasing the measurement
time t.

Example 20.6: An experimental neutron detector is under development that uses a semiconducting
compound with boron as a constituent in the form of B4 C. These films are usually grown on well-established
semiconductors such as Si. Because B4 C is difficult to produce, the layers are very thin. However, boron
is a p-type dopant in Si, and instead of a thin B4 C semiconductor detector, the device may actually be a
boron-coated pn-junction Si diode. For thin films, it is difficult to discern between the two possible outcomes.
Find an expression to determine the measurement time required to fulfill the desired confidence for any k
given a film thickness x and monodirectional thermal-neutron beam of intensity φn normally incident on the
film.

Solution:
The counts obtained in measurement time t from a bulk device should be
C2 = φn At (1 − exp[−xΣF ]) ,
where φn is the neutron flux intersecting the detector, A is the area, ΣF is the macroscopic cross section of
the film material, and x is the thickness. The counts from a coated device can be described by the ratio of
counts recorded from thin-film device to a that of a bulk device, namely
T F
C1 = φn At (1 − exp[−xΣF ]) ,
BK
where T F is the expected efficiency from the thin-film device and BK is the efficiency of the bulk device.
The difference between the two possible outcomes is
 
T F
C2 − C1 = φn At 1 − e−xΣF 1− = k (σT F + σBK ) .
BK
Square the expressions,
  2
T F
φn At 1 − e−xΣF 1− = k2 (σT F + σBK )2 .
BK
From this result the measurement time is found to be
* +
T F
1/2  1/2 2
−xΣF −xΣF
1−e + 1−e
k2 BK
t=   2 .
φn A T F
1 − e−xΣF 1−
BK
1094 Radiation Measurements and Spectroscopy Chap. 20

20.7.3 Coincidence and Anti-Coincidence Measurements


Detectors can be connected to interact together so as to record or reject events from radiation interactions.
For instance, two detectors may be connected in such manner that both must receive a radiation interaction
and produce a pulse within a certain time period Δt in order to record a count. Interaction events that do
not comply with this restriction are rejected. Such measurements are named coincidence counting. Further,
with spectrometers, an energy window can be used for one or more detectors to reduce the recording of
down-scattered or background gamma-ray coincidences. The opposite case can also be employed so that, if
two or more detectors record radiation interactions within a time Δt, all detectors reject the events. This
mode of operation is named anti-coincidence counting. The operation of such systems is summarized in
Chapter 21.

Compton Suppression
Compton suppression is an anti-coincidence method used to enhance the full-energy peaks in a gamma-ray
pulse height spectrum. In this method the gamma-ray spectrometer is surrounded by a second detector (or a
ring of detectors). For example, a HPGe detector is often used as the spectrometer, with a scintillator detector
(or detectors), formed into a ring around the HPGe detector, operated as a coincidence detector. Because
the total coincidence energy is of less concern than the recording of a full-energy event in the HPGe detector,
low-resolution scintillators with relatively high gamma-ray absorption efficiency are preferred (e.g., BGO
and NaI:Tl). With this configuration an incident photon that Compton scatters in the HPGe detector and
then escapes has a reasonable chance of subsequently interacting in the surrounding scintillation detector(s).
Both interactions occur at almost the same time. The partial photon energy deposited by the Compton
scattered photon in the HPGe detector can thus be suppressed by an anti-coincidence gate that accepts only
pulses in the HPGe detector that are anti-coincident with pulses in the scintillator(s). Thus, events in the
HPGe detector are recorded only if no simultaneous event occurs in the surrounding scintillator detector(s).
The resulting HPGe spectrum has a much reduced Compton continuum at all energies, thereby enhancing
the full-energy peak in the spectrum. Dramatic improvements in the pulse height spectrum can be achieved
[Molnar 2004; Bender et al. [2015]. Example spectra recorded with the technique are shown for LaBr3 :Ce in
Fig. 20.27 and HPGe in Fig. 20.28, both having an annular NaI:Tl guard detector for the coincidence gate
[Bender et al. [2015].
The Compton suppression method can be used to improve significantly prompt gamma-ray analyses.
Because prompt gamma rays tend to be of high energy (most are 1 < E < 12 MeV) there normally is a large
Compton component to the spectra, especially for relatively small semiconductor detectors. Suppression of
the Compton continuum with the anti-coincidence method, thus, produces a pulse height spectrum in which
full-energy peaks are more easily identified and quantified.

Positron Emission and Pair Production


Recall that when a positron comes nearly to rest, it combines with an electron to produce two 511-keV
annihilation photons. These 511-keV photons are emitted in opposite directions in order to preserve the
zero total linear momentum.11 If two detectors are placed on opposite sides of a source emitting positrons
isotropically (such as 22 Na), the two detectors can be connected such that a count is tallied only when both
detectors record a count within a small time interval Δt. The probability of recording a count is determined
by the geometry of the counting arrangement. Suppose that two cylindrical detectors with radii a1 and a2
are connected in coincidence and are placed opposite and at distances d1 and d2 from a positron source
with the cylindrical axes pointed at the source. The probability of recording a count is proportional to the

11 Very
rarely does the positron annihilate with an ambient electron before it has completely slowed. In this case the annihilation
gamma rays are not emitted in opposite directions.
Sec. 20.7. Experimental Design 1095

106 241
Am
60 keV
137
Cs ATM109 5mCi Unsuppressed
154
Eu 662 keV
ATM109 5mCi Suppressed
105 123 keV

104
154
Eu
723 keV
Counts

154
103 Eu 154
Eu
996 & 1005 keV 138
1274 keV La & 40K
1436 & 1460 keV

102

10

1
0 200 400 600 800 1000 1200 1400 1600
Energy (keV)

Figure 20.27. Unsuppressed and suppressed measured spectra from a 5 μCi ATM 109 spent fuel
sample using a LaBr3 :Ce-based Compton suppression system. From Bender et al. [2015]; courtesy
Kenan Ünlü, Penn State.

137
106 Cs
ATM109 5mCi Unsuppressed
241 662 keV
Am
60 keV ATM109 5mCi Suppressed
154
5 Eu
10 123 keV
134
134 Cs
Cs 154
10 4 605 keV Eu 796 keV
757 keV
154 154
Eu Eu 154
Eu
Counts

723 keV 996 & 1005 keV 1274 keV


3 154
Eu
{

10 873 keV

102

10

1
0 200 400 600 800 1000 1200 1400
Energy (keV)

Figure 20.28. Unsuppressed and suppressed measured spectra from a 5 μCi ATM 109 spent fuel
sample using an HPGe-based Compton suppression system. From Bender et al. [2015]; courtesy
Kenan Ünlü, Penn State.
1096 Radiation Measurements and Spectroscopy Chap. 20

smallest fractional solid angle12 Ωf for either detector, namely


   
1 d1 d2
Precord  1 2 min(Ωf 1 , Ωf 2 ) = 1 2 min 1−  2 , 1−  2 , (20.153)
2 d1 + a21 d2 + a22
where i i = 1, 2 is the detector gamma-ray interaction efficiency at 511 keV for detector i. Here it is assumed
that if one photon enters the detector with the smaller solid angle, then the other photon traveling in the exact
opposite direction must enter the opposite detector. However, any intervening material reduces this ideal
recording probability. The recorded pulse height spectrum consists almost entirely of a spectrum produced
by the 511-keV photons. The method almost entirely eliminates background, although the possibility of
accidental coincidence from background and other source emissions remains. Also, for example, with a 22 Na
source, the 511-keV annihilation spectrum would appear, but the 1.28-MeV gamma-ray spectrum would be
almost entirely absent, with perhaps a few counts from accidental coincidences.
Another radiation source that spontaneously emits two photons per decay is 60 Co; however, these gamma-
rays are randomly emitted in all directions. Using the same arrangement for coincidence counting with
identical detectors, the probability of a coincidence is now
Precord  1 Ω1 2 Ω2 , (20.154)
mainly because the two photons are not necessarily emitted in opposite directions and the solid angles of
both detectors must be taken into account. Hence, for radiation sources that emit more than one gamma ray
(e.g. 57 Co, 133 Ba), coincidence counting requires accounting for the solid angle of the two (or more) radiation
detectors as well as the branching ratios of the emissions. Shown in Fig. 20.10 are several sum peaks from a
60
Co source recorded with an HPGe spectrometer.
Positron
a Emission Tomography
An example of coincidence counting, which is widely used for medi-
cal imaging applications, is positron annihilation tomography (PET).
The system generally has a ring of individual detectors connected in
511 keV
coincidence as depicted in Fig. 20.29. The patient is administered a photon
positron emitting radiopharmaceutical, usually one of Na18 F, 82 RbCl, positron
annihilation
13
NH3 , or 18 FDG (fluorodeoxyglucose), which accumulates in the or-
gan or tissue under investigation. For instance, Na18 F accumulates in
bone tissue while 18 FDG accumulates rapidly in brain tumors. The patient

inoculated patient is passed through the detector ring, incrementally, detector


511 keV ring
in lengths more or less equivalent to the detector ring width. Annihi- photon
lation photons emitted from the patient may interact in two detectors
arranged in the ring about the patient, and through coincidence cir-
cuitry and ray tracing algorithms, the two detectors responding within
Δt to 511-keV annihilation photons can be used to identify a straight Figure 20.29. The basic layout for
line through the patient between the two detectors. An energy win- positron emission tomography.
dow can be set about 511 keV to help reject scattered photons and accidental coincidences. Although BGO
has been used in PET scanning systems, mainly because of its high gamma-ray absorption from Bi, the supe-
rior energy resolution of LSO, also having high gamma-ray absorption from Lu, is now used as a replacement
in most modern PET scanning systems. A backprojection algorithm is used to produce a three-dimensional
image of the patient, particularly the location where the positron emitters reside. An example of a PET
scan image is shown in Fig. 20.30.

12 The fractional solid angle is the solid angle subtended by a detector at the point source divided by 4π sr.
Sec. 20.7. Experimental Design 1097

Figure 20.30. PET images of a lymphoma patient. Left panel: prior to


chemotherapy. Right panel: two months post-chemotherapy. Illustration cour-
tesy of Dr. Frederic Fahey, Children’s Hospital, Boston, MA.

Phoswich Detector
The phoswich detector is a special scintillation spectrometer designed to measure low radiation levels in the
presence of high-energy ambient background radiation. The name comes from “phosphor sandwich”, where
two scintillation detectors are layered one atop
Scintillator
Housing the other [Wilkinson 1952]. The crystals are
Voltage
arranged as shown in Fig. 20.31, where light
Divider Base from both crystals is measured by a single pho-
Scintillator A tomultiplier tube. The signals from the different
(NaI:Tl) crystals are discerned by measuring the different
light decay times.
PMT The phoswich detector has a thin Be window
that allows the passage of low-energy photons.
Be window These low-energy photons can be absorbed in
the thin front detector, labeled A, which is de-
Magnetic signed to have sufficient thickness to absorb the
Optical
Shield radiation energies of interest, commonly on the
Scintillator B
(CsI:Tl) Window order of 1.5 to 3 mm thick. Higher energy pho-
tons generally pass through the front detector
Figure 20.31. The basic components of a phoswich detector. In
and can be absorbed in the much thicker back
this example, the front detector is a thin crystal of NaI:Tl, while the
back detector is a thicker slab of CsI:Tl. After Lindow et al. [1978]. detector, labeled B, commonly on the order of
50 mm thick. Pulse shape discrimination is used
to determine the pulses from different scintillators, which includes photons that Compton scatter from scin-
tillator B into scintillator A. Hence, pulses recognized as coming from scintillator A can be accepted while
those from scintillator B are rejected, thereby producing a spectrum primarily from only low energy pho-
tons. Coincident events from both scintillators can be rejected outright. Operated in anti-coincidence mode,
background events are substantially reduced. Consequently, the resulting spectrum has substantially re-
1098 Radiation Measurements and Spectroscopy Chap. 20

duced background so that low energy photon events can be seen. One interesting feature of this design is
that the signals are developed from a single PMT output. Coincident events are determined from pulses of
different rise times arriving within a preset time window. Detectors for low-energy gamma rays commonly
have combinations of either a thin NaI:Tl crystal upon a thicker CsI:Tl crystal, or a thin CaF2 :Eu crystal
upon a thicker NaI:Tl crystal. Other combinations have been explored, which for example include the use
of BGO, GSO, and BaF2 in various combinations [Costa et al. 1986; Kamae et al. 1993; Futami et al. 1993].
The use of YSO with LSO and LuYAP with LSO has also been explored for positron emission tomography
applications [Dahlbom et al. 1997; Eriksson et al. 2013].
Although phoswich detectors are often designed for low-energy gamma-ray and x-ray detection, they have
also found use with charged particle detection [de Celis et al. 2007]. For instance, the combining of ZnS:Ag
as a thin front detector with an organic (plastic) scintillator as a back detector, alpha particle events can
be separated from beta particle events [Usuda 1992]. Recall from Chapter 13 that ZnS:Ag is used for heavy
particle detection, but is inefficient as a gamma-ray or electron detector. Hence, alpha particles can lose all
energy in the thin ZnS:Ag front detector (usually only tens of microns thick), while the back detector can
absorb the full electron energy. The small amount of energy deposited by electrons in the front detector is
negligible. Hence, the particle counts can be separated by either pulse shape or pulse height discrimination.
Note that the same method can be used to discriminate gamma rays and charged particles from neutrons,
where neutrons slip through the first detector (low cross section) and scatter in the second (organic scintil-
lator) [Watanabe et al. 2008]. If the first detector has adequate gamma-ray and charged-particle interaction
efficiency, coincident events can be rejected while recognizing neutron scatters in the second detector.
Special designs with fast (front) and slow (back) plastic scintillators are used for particle energy spec-
troscopy and identification [Wilkinson 1952; Bodansky and Eccles 1957; Saint-Gobain 2019a]. Particles
passing through the first detector (fast response) yield information about the stopping power, or dE/dx,
while summing the total integrated light from both detectors yields the particle energy.

Anger Camera
The Anger camera, or gamma-ray camera, was introduced by Hal Anger [Anger 1958]. A cross section of
the basic components of the device is depicted in Fig. 20.32. The device can be used with single photon
emission computed tomography (SPECT) or PET. The system consists of an array of photomultiplier tubes
populated upon a thin sheet of NaI:Tl scin-
tillator. The scintillator is usually on the or- gamma rays lead
der of 6 mm to 12 mm thick. The patient is collimator
administered a radiopharmaceutical, commonly
containing 99m Tc which emits 140-keV gamma diffuse
rays, and placed adjacent to the Anger camera. reflector
Other radiopharmaceuticals used for SPECT in- scintillator
photons coupling grease
clude 123 I (159 keV) and 111 In (mainly 23 keV,
171.3 keV, and 245.4 keV, although there are light pipe
other emissions). Gamma-ray photons emerg-
ing from the patient can be absorbed in the rel- PMT array
atively thin NaI:Tl scintillator, spontaneously shielding
producing scintillation photons emitted isotrop-
ically. To reduce the measurement of scattered readout
electronics
gamma rays, which can blur the image and
produce an erroneous correlation to the emis- Figure 20.32. The basic components of a gamma-ray camera
sion point, a collimator is aligned in front of (Anger camera).
the NaI:Tl scintillator. The collimator also im-
Sec. 20.7. Experimental Design 1099

Eg Det 1 dN
dE

collimators q

E’
g
Det 2 Det 1
Det 2 E
Figure 20.33. Geometry for a Compton spectrometer, in which detector 1 and detector
2 are operated in coincidence. The dotted line spectrum represents the energy spectrum
absorbed in detector 1, while the shaded spectra represent the coincident energy spectra
recorded by either detector 1 or detector 2 (as indicated).

proves the spatial resolution, but consequently also greatly reduces the detection efficiency. Multiple PMTs
are usually involved with measuring the light and the closest PMT to the gamma-ray event produces the
largest voltage signal. An algorithm weights the different PMT signals in the x and y directions and en-
sures the signals arrive within some Δt coincidence time interval to be included in the measurement. This
algorithm was originally a clever resistor circuit capable of identifying the interaction location within 5 mm.
Advanced electronics and algorithms in modern Anger cameras can reproduce the interaction location with
spatial FWHM of 3 mm [Cherry et al. 2003).
Compton Spectrometer
A Compton spectrometer is a coincidence mode device used to extract information from the combination of
two or more detectors. The basic geometry of the method is depicted in Fig. 20.33. Two radiation detectors
are connected in coincidence, with one acting as the main detector (detector 1, for example) and the second
detector acting as the coincidence witness. A collimator is used for detector 1 and also (preferably) detector
2, to narrow the directions of both the initial and scattered gamma rays. Sometimes a narrower witness
detector is used instead of the collimator for detector 2. The geometric arrangement is important, because
detector 2 is set at a specific angle θ with respect to the collimated gamma-ray trajectory.
The Compton spectrometer is a method, albeit inefficient, originally intended to produce a gamma-
ray spectrum from counters instead of spectrometers. Obviously, the energy resolution depends on the
uncertainty in the scattering angle. Hence, better collimation of both the initial gamma-ray and the Compton
scattered gamma-ray decreases this uncertainty, but it also reduces the efficiency and, consequently, requires
an increased measurement time. Gamma rays absorbed in the first detector by the photoelectric effect do
not produce a coincidence event with the witness detector and are excluded. The method can be used to map
out the Compton continuum, the Compton edge energy yielding the initial gamma-ray energy. Yet, there
is still the possibility that multiple Compton scatters occur in detector 1, with the final scattered photon
emerging and still producing a coincidence in detector 2, giving a false indication of the original gamma-ray
energy. This problem can be reduced by using smaller detectors or replacing the counters with detectors
capable of spectroscopy.
Compton Spectrometer for Light Yield Measurements In Figs. 13.4 and 13.5, it is seen that many
scintillators have non-linear light yields for electron energies below about 500 keV, i.e., the emitted light
is not proportional to the electron energy deposited in the scintillator. One method to measure the light
yield as a function of energy deposition is to measure directly the light yield with multiple gamma-ray
sources, preferable monoenergetic sources. However, this method relies, in practice, on only a few sources
and, thus, leaves wide energy gaps in the measurements. A type of Compton spectrometer can be used
1100 Radiation Measurements and Spectroscopy Chap. 20

to measure the light yield of scintillators over a much larger range of deposition energies than possible
with common monoenergetic gamma-ray sources [Valentine and Rooney 1994]. This device is a regular
Compton spectrometer, shown in Fig. 20.33, with the change that the first detector is now made from
the scintillation material being studied and the second detector is a gamma-ray spectrometer. A known
monoenergetic gamma-ray source, 137 Cs for instance, is used to irradiate the test scintillator (detector 1).
Scattered gamma-ray events in detector 2 are tallied in coincidence with events in detector 1. The energy of
the scattered gamma rays is known from the collimated scattering angle. At the same time the light yield
from the test detector is measured with a photomultiplier tube. With this technique the light yield for many
different deposition energies, determined by the scattered photon energies (Eγ − Eγ ), can be measured using
the same monoenergetic source by simply changing the coincidence scattering angle.
Also designed for light yield measurements, a relatively complicated Compton coincidence spectrometer
system was reported, named the SLYNCI for Scintillator Light Yield Non-proportionality Characterization
Instrument, with five HPGe detectors connected in coincidence with the test scintillator [Choong et al.
2008]. This device still requires source collimation between the source and the test scintillator, although no
collimators are used between the test scintillator and the multiple HPGe coincidence detectors. The SLYNCI
system was designed to reduce the measurement time required to characterize the light yield from a test
scintillator.
The design of the Compton coincidence light yield system was significantly simplified by Ugorowski et al.
[2008] by placing a small gamma-ray check source adjacent to the test scintillator and using a high-resolution
HPGe detector for the coincidence witness detector. Because there are no collimators in this design, the
HPGe detector is placed near the test scintillator, thereby increasing the solid angle of the witness detector.
These three simple design changes remove the need for any collimators, decrease the uncertainty in the
measurement, and reduce the measurement time. This simpler arrangement also negates the need to know
the Compton scattering angle because the HPGe detector provides the residual energy, from which the energy
deposited in the test scintillator can be inferred.
Compton Camera System The Compton imaging system also depends on the properties of photon scat-
tering to locate gamma-ray sources. The basic device has a position sensitive front detector following by
another position sensitive back detector [Schönfelder et al. 1973]. The device is designed so that some gamma
rays scattered in the front detector are subsequently absorbed in the back detector. The two detectors are
operated in a coincidence mode to ensure that scattering and absorption events are correlated. Because this
system does not require a collimator, the overall gamma-ray detection efficiency is improved compared to
gamma-ray cameras that require collimators to exclude background. In this device the location of where an
incident gamma ray interacts in the first detector and the location of where the scattered photon is absorbed
in the second detector are measured, within the spatial resolution limits of the front and back detectors, and
a ray can be traced between the two interaction locations.
If the incident gamma-ray energy is known, the energy deposited in the first detector and the interaction
locations in both detectors can then be used to extract information about the location of the gamma-ray
source. From the Compton scattering condition of Eq. (4.32), the energy deposited in the first detector is
 
Eγ (1 − cos θ)
Ee = Eγ − Eγ = Eγ . (20.155)
511 keV + Eγ (1 − cos θ)

The direction of the scattered gamma ray is traced between the two interaction positions in the two detectors.
Hence, Eγ and Ee are both known, leaving θ as the only unknown. This angle θ can be reconstructed as
a cone with the surface forming all possible directions as depicted in Fig. 20.34(a) [Everett et al. 1977].
A second gamma-ray scatter produces a new angle, depicted as φ in Fig. 20.34(b), and a new cone is
reconstructed, overlapping the first cone in two locations. After several additional cones from more gamma
Sec. 20.7. Experimental Design 1101

reconstructed det 1
cone

q
f

source det 2
source
(a) (b)
Figure 20.34. The Compton camera concept; detector 1 is the position sensitive scatter
spectrometer; detector 2 is the position sensitive absorber detector. (a) A reconstructed
cone with angle θ from a Compton scatter. (b) Another reconstructed cone with angle φ.
The cone perimeters overlap at the source location.

rays are reconstructed, a specific location where all of the cones overlap becomes apparent and so the source
location is identified. The method becomes more complicated if multiple sources are in the field of view.
However, the reconstructed cones can still image the location of these sources because the images increase
at the multiple crossover points.
If the energies of the gamma rays emitted by the source are not known a priori, then, with Eγ unknown,
the scattering angle θ cannot be calculated from Eq. (20.155). However, this problem can be overcome
by using a position-sensitive high-resolution gamma-ray spectrometer as the second detector. The sum of
energies deposited in the first and second detectors can then be used to determine Eγ , preferably with
the scattered gamma ray completely absorbed in the second detector by the photoelectric effect. The
weakness of this approach is that the Compton scattered gamma ray may not be completely absorbed in the
second detector but instead be scattered out of it. This incomplete energy absorption leads to an erroneous
estimation of Eγ . The probability of fully absorbing the scattered gamma ray is improved if the second
detector is made from high Z materials. Also, the device thickness can be increased with the consequence
that multiple scatters may occur in the second detector, thereby confusing the interaction location. Another
remedy is to use multiple stacked position sensitive spectrometers as scatter planes to back trace the gamma-
ray path, ultimately producing a reconstructed cone that intercepts the source location(s) [Dogan et al. 1990].
Also, an anti-coincidence detector surrounding or near the Compton camera can eliminate a significant
number of events when the scattered gamma rays escape the system [Dogan et al. 1990].
Compton Spectrometer and Imager The Compton spectrometer and imager (COSI) is a Compton camera
instrument designed for the study of astronomical gamma-ray bursts [Lowell et al. 2016, 2017]. It has a 2
× 2 × 3 position-sensitive array of double-sided HPGe strip detectors [Amman et al. 2007] operated in
coincidence as a Compton camera with an additional CsI:Tl scintillator shield surrounding the array that
operates in anti-coincidence to reduce background [Kiernans et al. 2016]. The CsI:Tl shield rejects escaping
Compton scattered gamma rays that interact in the shield so they are not used in the estimation of the
incident gamma-ray energy. The shield also passively and actively blocks albedo radiation and vetoes high-
energy charged particles. The position resolution of the HPGe strip detectors is reported to be 2 mm in the
x and y directions and approximately 0.2 mm in the z direction. Designed to detect gamma rays between
200 keV to 5 MeV, the FWHM energy resolution of the COSI is 2.7 keV at 661.7 keV. The detector is kept
cool with a mechanical Stirling cycle cryocooler. The device is deployed on a high pressure balloon, complete
with solar panels to maintain power. When deployed, the COSI field of view is approximately 25% of the
1102 Radiation Measurements and Spectroscopy Chap. 20

sky. In at least one launch, the COSI stayed aloft and collected gamma-ray data for 46 days [Kiernans et al.
2016].
Portable Compton Scatter Cameras There are portable variants of the Compton camera used mainly as
gamma-ray imagers and source identifiers. These detectors are used to rapidly locate gamma-ray sources in
a region and often need only a few dozen interactions to locate the sources. A relatively complex Compton
scatter camera is the position sensing CdZnTe gamma-ray spectrometer, named the Polaris spectrometer
[Wahl et al. 2015; H3D 2018]. This device has various numbers of position sensitive CdZnTe spectrometers
arranged in layers of arrays. Each CdZnTe detector can sense the interaction position within the detector
volume using a depth sensing technique based on a pixelated electrode configuration.
A gamma-ray camera with dual capability as a Compton scatter camera and a pin-hole camera is reported
by Hull et al. [PHDS 2018]. The detector, named GeGI for germanium gamma-ray imager, has a single
slab of pixelated HPGe attached to a Stirling cycle mechanical cryocooler. The 9-cm diameter and 1-cm
thick spectrometer is a position sensitive strip detector, with strip pitches of 5 mm. Instead of several
detectors operating as scatter and absorption spectrometers, the GeGI operates by position tracking the
signals produced within separate pixels formed by the x and y positions of the strips. The z direction is
inferred from the charge collection signal by using the three dimensional sensing system developed by He
and Zhang [2008].
A scintillation Compton camera alternative is a device built with GAGG:Ce scintillators [Kishimoto et
al. 2014; Kataoka et al. 2018]. The GAGG:Ce Compton camera is based on the original concept proposed by
Schönfelder et al. [1973], in which two arrays of position sensitive scintillators are aligned as the scatter and
absorption spectrometers. The three-dimensional sensing device is constructed with individual GAGG:Ce
scintillators, with nominal dimensions of 2 mm × 2 mm × 4 mm, arranged in 11 × 11 pixel arrays. The
scintillators are separated by reflectors and have multi-pixel photon counters (MPPC, alternatively named
SiPMs) attached to both sides. Both the scattering plane and the absorbing plane have four scintillator array
blocks each separated by 12 mm. The x and y interaction positions are determined by the location of the
affected pixels while the z component is determined by pulse height ratios measured with the dual MPPCs.
Although the energy resolution (∼ 8.6% FWHM at 661.7 keV) is not as good as the CdZnTe and HPGe
counterparts, the device is relatively lightweight (∼ 1.9 kg) and provides an angular resolution of about 8◦
to 9◦ FWHM.

20.8 Gamma-Ray Spectroscopy—Summary


Gamma-ray spectroscopy seeks to determine, first, the gamma-ray energies emitted by radionuclides (which
emit gamma rays of distinct energies) that are present within a sample. This goal can be called qualitative
analysis. However, generally, one also seeks either the source strength of the particular gamma rays or the
concentration of the radionuclide emitting the gamma rays. This more demanding task often is referred to
as quantitative analysis.
The objectives of gamma-ray spectroscopy are realized by analyzing the pulse height spectra. In this
chapter, pulse-height spectra in which the number of counts are specified by discrete channel number are
considered. This approach is used because channel number is directly proportional to pulse height and, thus,
to the photon energy deposition. Consequently, quantitative information can then be obtained from the
pulse height spectrum whether or not the spectrometer is linear. Spectroscopic analysis techniques begin by
attempting to determine the continuous channel number that corresponds to the centroids of the full energy
peaks in the spectrum that are of interest. The MCLLS approach focuses on the entire spectrum and seeks
to determine the parameters of models that best fit all or major portions of the spectra. The symbolic Monte
Carlo approach holds promise for spectroscopic applications in which the model is non-linear in terms of the
radionuclide concentrations of samples.
Sec. 20.9. Charged-Particle Spectroscopy 1103

Depending upon the need, there are several devices that can be used for gamma-ray spectroscopy. Effi-
ciency with adequate energy resolution can be provided with large volume scintillators, whereas high energy
resolution can be achieved with semiconductor detectors. Both scintillator and semiconductor detectors can
be acquired as portable units with good detection efficiency for gamma rays. For ultra-high energy resolution,
microcalorimeters or WDS diffractometers offer excellent performance (as described in Chapter 19). Yet,
microcalorimeters and WDS spectrometers are generally restricted to laboratory-based instrumentation for
low energy gamma rays and x rays. Note that the spectrometers discussed in the present chapter represent
only a select sample of variations that are commercially available. More information can be found in earlier
chapters dedicated to semiconductor and scintillation detectors.

20.9 Charged-Particle Spectroscopy


With charged-particle spectroscopy it is possible to identify some radioisotopes, provided that certain ex-
perimental precautions are exercised. As charged particles travel in a medium, they lose energy, mainly
through Coulombic interactions. The amount of kinetic energy lost depends on the material stopping power,
the particle energy, and the particle mass and charge. Regardless, energy is lost, even if the particle is
emerging from its own source material. If some small and variable energy is lost before the particle enters
the active region of the detector where it is subsequently stopped, the measured deposited energy is not
the initial energy of the particle. Consequently, the uncertainty in the energy of a particle is increased and
the energy resolution of the spectrometer decreases. To reduce energy losses while improving energy reso-
lution, charged-particle measurements of relatively small samples are often conducted in a vacuum. Sample
preparation is also important to ensure the mass thickness of a laboratory sample is kept relatively low so
as to reduce energy self-absorption losses. It is also important to reduce the mass thickness of any material
between the source and detector.

20.9.1 Electrons, Positrons, and Beta Particles


 Electron, conversion electron, positron, and beta par-
ticle spectroscopy can all be conducted with organic
  



and liquid scintillation counters; however, the preferred

method to achieve high-energy resolution is to use low Z
semiconductor detectors, mainly Si detectors. The rea-
 

  son for low Z materials becomes evident from Fig. 7.7


in which it is seen that the backscattering of electrons
 and beta particles from a material increases with atomic
number. The electron backscatter coefficient ranges be-

tween 0.14 at 50 keV down to 0.06 at 2 MeV, reducing to
0.0125 at 10 MeV. Any variety of planar Si detector can

 
 
 
 
 
  detect electrons, yet because the range of electrons can
     be significant (see Fig. 4.23 and Fig. 20.35), the type of
detector is important. For instance, the mass thickness
Figure 20.35. Average electron range in Si as a function
of energy. Data are from ESTAR [NIST 2018]. range for 100 keV and 1 MeV electrons is 0.018 g cm−2
and 0.54 g cm−2 , corresponding to ranges in Si of 77 μm
and 2.36 mm, respectively. In the former case, a silicon surface barrier or implanted junction detector can
be depleted, with reasonable voltage, to absorb all energy. However, the latter case would require excessive
voltage to achieve a 2.31-mm-thick depletion region, and it would be better to instead use a Si(Li) detector.
Note that the trajectory of electrons in a solid undergoes significant scattering as shown in Fig. 4.22. Hence,
1104 Radiation Measurements and Spectroscopy Chap. 20

it is still possible to absorb the total electron energy in the detector even if the active thickness is somewhat
less than the average linear range.
To preserve the electron energy distribution of the source, the measurement should be conducted in a
vacuum. Such a measurement is straightforward for SSB and pn junction detectors, but Si(Li) detectors are
often cooled during operation and, hence, require encapsulation to prevent contamination. Consequently,
the use of a Si(Li) detector for low-energy electron spectroscopy requires a thin, low Z, window (such as
Be) and the ability to produce a vacuum between the detector window and the source. Ahmad and Wagner
[1974] describe a Si(Li) detector operated in vacuum with apparently no window between the source and
detector face, although there was a 2-micron-thick contact layer.13
The pulse height energy deposition of monoenergetic electrons in Si was studied by Berger et al. [1969a]
who compared Monte Carlo calculations to measured energy spectra. A few of their comparisons are shown
in Fig. 20.36. Three detector types were used (of six different thicknesses) for the measurements, including
silicon surface barrier (SSB) detectors, a diffused junction detector, and Si(Li) detectors. In Fig. 20.36 (left
column), different detectors were used to measure 250-keV electrons with an average range of 343 microns
in Si. Although the 105-micron-thick detector was less than the electron range, some scattered electrons did
deposit their full energy in the detector. The full energy peak also appears in the two thicker detectors. In
Fig. 20.36 (right column), the detectors were used to measure 1-MeV electrons (range of 2.36 mm). These
electrons pass through the SSB detector, depositing only a fraction of their energy. The thicker diffused
junction detector does show a full energy peak, but of low efficiently. The thicker 3 mm Si(Li) detector
showed a significant full energy peak. Detailed response functions and range tables for electrons in Si
detectors can be found in the literature [Berger et al. 1969b].
A low-energy tail, a consequence of partial energy deposition in the detector, usually appears, regardless
of detector thickness. For relatively thin detectors, electrons may pass directly through the device and leave
only a fraction of energy, as shown in Figs. 20.36(a, left and right). Backscatter losses can also cause partial
energy deposition, as shown in Figs. 20.36(b,c left and right). Self-absorption energy loss as electrons or
beta particles emerge from a sample, or energy attenuation between the sample and detector active volume,
are other sources of energy loss that can contribute to the low-energy tail. The angle that electrons enter
the detector can also cause a difference in backscattering, increasing as the angle increases from that of
normal incidence. Also, the escape of characteristic and bremsstrahlung x rays may contribute to the energy
loss tail. For positron detection, there is a small chance that 511-keV annihilation photons emitted from
the eventual recombination of an electron and positron may simultaneously deposit some (or all) energy in
the detector, thereby producing a high-energy tail above the full-energy positron peak. Measured response
functions for monoenergetic electrons and positrons were reported by Frommhold et al. [1991] and compared
to Monte Carlo simulations. The basic components of a monoenergetic electron or position spectrum are
identified in Fig. 20.37(left). Unlike an electron spectrum, a positron spectrum has a high-energy tail above
the full energy positron peak as a result of the Compton scatter of 511-keV annihilation photons.
Additional distortions of the true electron energy distribution arise from detector and electronic effects.
If T (E) is the number of electrons, per unit energy, incident on the detector, the measured energy deposition
M (E  ), per unit energy, in the detector by these electrons is

 ∞
M (E  ) = R(E, E  )T (E) dE, (20.156)
0

13 The authors refer to the Au contact as a window, but this is traditionally improper nomenclature. Such contacts are usually
referred to as “dead layers.”
Sec. 20.9. Charged-Particle Spectroscopy 1105

 
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Figure 20.36. Comparison of Monte Carlo calculated and measured pulse height spectra for (left
column) 250-keV electrons and (right column) 1-MeV electrons for different Si detector thicknesses: (a)
105-μm SSB detector; (b) 530-μm diffused-junction detector; (c) 3-mm Si(Li) detector. The points are
experimental and the lines are calculated results. Data are from Berger et al. [1969a].
1106 Radiation Measurements and Spectroscopy Chap. 20

10   
(a)
 

full energy
Counts (arbitrary units)

8 transmission peak
peak


6


4
back- Bremsstrahlung  

scattering loss tail Compton


2 loss tail
scattering

0 
0 2 4 6 8 10    

Energy (arbitrary units)  

Figure 20.37. (a) Response function components of a monoenergetic electron or positron spectrum (after Frommhold
et al. [1991]). The Compton scattering distribution from 511-keV annihilation photons is absent from an electron
spectrum. (b) A measured positron spectrum compared to a Monte Carlo calculation. Data are from Frommhold et
al. [1991].

where R(E, E  ) is the detector response function normalized such that


 ∞
R(E, E  )dE  = 1. (20.157)
0

Tsoulfanidis et al. [1969] developed the following response function to describe the energy deposition E  by
monoenergetic electrons of energy E in a plastic scintillator:

b E − E 1−b −(E − E  )2
R(E, E  ) = 
erfc √ + √ exp (20.158)
2E σ 2 σ 2π 2σ 2
where the complimentary error function is
 z
2
erfc(z) = 1 − √ exp(−t2 )dt, (20.159)
π 0

σ is the standard deviation of the modeled Gaussian function and b is the fraction of electrons appearing in
the tail region,
√ g σ
b−1 = 1 + 2π − 0.5 , (20.160)
t E
where g is the height of the full energy peak and t is the height of the backscattering tail region. The energy
response function for beta particles with their continuous energy distribution is certainly more complex, but
can be addressed by dividing the beta source spectrum into energy groups. The matrix of response functions
can then be used to unfold energy deposition spectral data. For instance, beta particle spectra have been
produced from pulse height energy deposition spectra acquired with scintillators and Si(Li) detectors with
the use of unfolding methods [Tsoulfanidis et al. 1969; Dakubu and Gilroy 1978].

20.9.2 Alpha Particles


The best detectors for alpha particle spectroscopy are low-Z semiconductor detectors such as SSB and
implanted junction Si detectors. The range of most alpha particle emissions from calibration check sources is
Sec. 20.9. Charged-Particle Spectroscopy 1107

less than 60 microns in Si, which is a depletion region thickness that can be produced in SSB and implanted
junction detectors with a reasonable voltage. With very pure Si, the width of the depletion region may be
sufficiently wide from just the junction potential (Vbi ). However, it is recommended that reverse voltage be
applied to improve charge collection and reduce detector capacitance.
Because each alpha particle emission is monoenergetic, although some sources have multiple alpha particle
emission energies, the general expectation is the formation of a Gaussian full-energy peak for each alpha
particle energy. However, the full-energy deposition peak usually is not perfectly Gaussian for several reasons.
First, the variance is actually less than that predicted with Poisson or Gaussian statistics because the FWHM
with units of energy must be corrected with a Fano factor F as
 
FHWM = 2 2 ln(2)Eα wF = 2.355 Eα wF , (20.161)

where w is the average ionization energy and Eα is the alpha particle energy. The Fano factor for Si is
generally quoted to be about 0.115 (see Table 16.2).
Second, a low-energy tail inevitably appears in the energy-deposition spectrum because some of the
alpha particle’s initial energy is lost as a result of self-absorption as the particle emerges from the source
material and also as the particle passes through the detector dead layer. The energy loss from the source
self-absorption and detector dead layer also decrease the energy resolution. Another contributor to the tail
arises from backscattering of the alpha particle which varies with the incident direction of the particle on the
detector although this backscatter effect is usually minor [Bertolini and Coche 1968]. Backscattering and
attenuation effects were addressed in Sec. 7.2.1. As is observed in electron and positron energy-deposition
tails, escaping x-ray emissions from excited electron states produced by the passage of alpha particles in the
detector material may also contribute to counts in the spectral tail. Alpha particles can also backscatter
from the source backing. Consequently, the count rate recorded by an alpha particle detector may need
several corrections to account for the many contributors of the low energy tail.
Third, the value of mean ionization energy w is usually somewhat greater for alpha particles than that
for gamma rays. The reason for this difference is that alpha particles have sufficient energy and mass to
cause nuclear recoil events in Si, events which do not produce electron-hole pairs. Consequently, there
is an additional source of variance in the pulse height spectrum from the distribution of Si recoils, along
with a reduction in the total number of charge carriers produced. Bertolini and Coche [1968] estimate this
contribution to the energy resolution is about 6 keV for 5-MeV alpha particles. Fourth, although Si is a
mature semiconductor, some part of the low-energy tail may be a consequence of incomplete charge collection
[Steinbauer et al. 1994].
Finally, at certain orientations, ions can enter the semiconductor crystal and pass between adjacent
atomic planes, an effect called channeling. The consequences of channeling include extended ion ranges
and reduced linear energy transfer (LET or stopping power) [Gibson 1965]. Channeled alpha particles can
have significantly longer ranges than those shown in Fig. 4.23. Hence, channeling alpha particles may pass
well beyond the depletion region, thereby depositing only a fraction of their energy in the active region of
the detector [Dearnaley 1964] and producing counts only in the low-energy tail region. The LET is lower
for channeled alpha particles, and thin transmission detectors designed for dE/dx measurements produce
incorrect results [Madden and Gibson 1964]. Channeling also has an effect on detector fabrication in which
ion implantation is used to introduce dopant impurities to form a pn junction. The actual junction depth
increases beyond the predicted depth, producing a much thicker surface dead layer. Detectors are usually
oriented at a slight angle from normal towards the source to prevent channeling.14 There is a critical angle
θc from a major crystal plane beyond which channeling is negligible [Seidel 1983] and, for heavy ions, is

14 Semiconductor wafers are usually oriented between 7◦ to 11◦ from normal to the ion trajectories.
1108 Radiation Measurements and Spectroscopy Chap. 20

calculated as [Morgan 1973]


 1/2
2Z1 Z2 qe2
θc = radians, (20.162)
Ed
where Z1 is the ion, Z2 is the target material, qe is the fundamental electronic charge, E is the particle
energy, and d is the interplane spacing along the channeling direction. The transition between high and low
energy ions is generally defined by
2dZ1 Z2 qe2
E , (20.163)
a2
where a is the Thomas-Fermi screening radius in angstroms
−1/2
2/3 2/3
a = 0.8853 a0 Z1 + Z2 , (20.164)

where a0 is the Bohr radius of 0.529 Å (5.29 nm). For low-energy ions, the critical angle is [Middleman and
Hochberg 1993]
*√ +1/2
3a
θcL = √ θc radians. (20.165)
2d
It turns out for Si, the transition energy for alpha particles defined by Eq. (20.163) is 104.4 keV. Alpha
particles are invariantly emitted at higher energies than 100 keV, hence the use of Eq. (20.162) is appropriate
for alpha particle spectroscopy with Si detectors.
The response signal from protons and alpha particles is linear for semiconductors in the absence of heavy
charge carrier trapping. Deviations from linearity may be a consequence of energy loss in the contact dead
layer, recombination of electron-hole pairs (especially near the end of the particle range), trapping, and
nuclear recoils. Energy calibration with zero offset can be accomplished with the assistance of spectrometer
grade check sources (see Sec. 20.5.1). There are some alpha particle sources of special interest for calibration
purposes, including 241 Am, 148 Gd, 226 Ra, and 228 Th. Perhaps one of most used calibration sources is
241
Am, mainly because of its long half-life (432.7 years), average emission energies, and absence of interfering
radiations, save for a 59.5-keV gamma-ray emission and some Np x-ray emissions at low energies. Although it
appears to be monoenergetic, it actually has five energy emissions, all near 5.5 MeV [Chanda and Deal 1970].
When operated in vacuum with a well-prepared source, surface barrier and implanted junction Si detectors
with excellent energy resolution can resolve all five emissions. However, usually only four alpha-particle
emissions are discernible (see Fig. 16.12).
The 148 Gd source is of special interest for two main reasons: it is truly monoenergetic with a (relatively)
low-energy alpha-particle emission of only 3.18 MeV and it has a comfortably long half-life of 70.9 years.
148
Gd has at times been difficult to acquire, mainly because it is a spallation byproduct from accelerator
targets that are not always available.15 Two sources with relatively high-energy alpha-particle emissions are
226
Ra and 228 Th. Both of these sources emit multiple alpha-particle energies from daughter products. 226 Ra
has a half-life of 1599 years, with its highest energy emission being from daughter 214 Po of 7.69 MeV (see
Fig. 16.12). However, a daughter product is also 222 Rn, which emits a 5.49-MeV alpha particle. Because
222
Rn is a gas, this daughter product can diffuse from the source and contaminate the detector, causing
the appearance of a background peak. Fortunately, the half-life of 222 Rn is only 3.82 days and almost all
daughters in the chain also have short half-lives; hence the background peak disappears after a few weeks.
Regardless, for measurements requiring a low background environment, the operator may wish to avoid using

15 It took over five years of waiting for the authors to get a spectroscopic grade 148 Gd source.
Sec. 20.9. Charged-Particle Spectroscopy 1109

this source with a dedicated low-background detector. 228 Th has a relatively short half-life of only 1.91 years.
228
Th, with daughter products, is also a multi-energetic alpha-particle emitter. The highest emission energy
is 8.78 MeV from daughter 212 Po, amongst one of the highest alpha-particle energies available as a check
source.

20.9.3 Heavy Ions


Heavy ions, such as fission fragments, generally do not produce a linear spectrometer response. Instead,
there is a marked signal loss with heavy ions, i.e., they produce a significantly smaller signal than that
predicted for lighter ions of the same energy [Schmitt et al. 1965]. This difference in the expected and the
observed results is called the pulse height defect (PHD) [Miller 1961]. The specific energy loss is highest
for heavy charged particles at the entrance point in the detector, quite the opposite of alpha particles and
protons which have their highest energy loss at the end of their paths as shown in Fig. 4.28. Consequently,
energy loss in the dead layer of the detector is higher for heavy charged particles than that observed for
alpha particles and protons. As is well documented, the pulse height defect can be sizeable for heavy ions
[Bertolini and Coche 1968] and is reported to be between 10±3 MeV to 20±3 MeV [Miller 1961; Finch 1973].
A measurement method used to reduce the
effect of PHD is the time-of-flight (TOF) tech-

nique, briefly mentioned in Sec. 17.10 for ther-
  
 !   mal neutron detectors. However, a thin zero
" !  
time detector is used to discern the timing start

condition instead of a “chopper”, while a second
  

 detector is used to define the transit time and


(with limited resolution) particle energy. A par-

ticle passing through the zero time detector trig-
 gers the start time, while the second detector de-
termines the stop time or t and residual energy

E  . The zero time detector may be active or pas-
 sive. In the passive case, the ion passes through
a thin window (e.g., polymer or carbon film)

     that causes the emission of electrons [Fraser and
Milton 1958; Milton and Fraser [1962]; DiIorio
      
and Wehring 1977], and these electrons are then
Figure 20.38. Fission fragment energy distribution for (–) time-of- deflected into a detector that provides the fis-
flight before neutron emission, (- -) time-of-flight after neutron emis- sion fragment start time. A simple active zero
sion, and (•) data from an SSB detector. Data are from Kobayashi time detector is a thin ΔE device, such as a thin
et al. [1965].
gas-filled detector, a thin plastic scintillator, or
a thin fully depleted SSB detector. Knowledge of the travel distance provides the velocity, while the sum of
E  + ΔE provides energy, or
2(E  + ΔE)t2 2Et2
M= 2
= 2 , (20.166)
d d
where d is the distance between the detectors and M is the particle mass. If ΔE is negligible, then E  E  .
Time resolution is usually on the order of 250 ps or less, and the uncertainty in timing can be decreased by
increasing t (i.e., the transit distance) [Butler et al. 1970; Zeidmen et al. 1974]. Hence, timing resolution
can be designed to contribute less than 0.1% to the overall measurement uncertainty. Consequently, it is
the energy resolution that strongly affects the mass resolution. Because fission fragments are emitted with
various charge states, the energy resolution of the stop detector is limited. For example, an SSB detector
1110 Radiation Measurements and Spectroscopy Chap. 20


  


 


 
 
!

     

 

Figure 20.39. Actual ion energy versus pulse height channel number for a
few heavy ions measured with an SSB detector. Data are from Wilkins et al.
[1971].

is limited to 2%–4% FWHM for fission fragments. DiIorio and Wehring [1977] use an electrostatic analyzer
between the zero time detector and an SSB stop detector to sort different kinetic-energy-to-ionic-charge
ratios, and, thereby improve the particle mass resolution to less than 0.5 amu.16 A comparison of the energy
measured for fission fragments using time-of-flight methods and an SSB detector is shown in Fig. 20.38.
The solid curve depicts the energy distribution of fission fragments before prompt neutron emission, the
dashed curve depicts the energy distribution of fission fragments after prompt neutron emission, and the
data points were collected by the Si detector (after prompt neutron emission). The PHD is clearly shown
by the difference with the SSB detector response and the time-of-flight responses.
However, the high energy loss from source self-absorption and dead layer losses (nominally only about
2 MeV) are not the only loss mechanisms. Dearnaley and Northrop [1966] emphasize that non-ionizing
nuclear recoils (in Si) are a major source of energy loss that contributes to the PHD. There are even more
mechanisms that contribute to the PHD. These include electron and hole recombination in the dense charge
cloud produced by the heavy charged particles. Also charge carriers are lost by being trapped in crystal lattice
defects, an effect which increases as the semiconductor is exposed to increasing numbers of heavy particles.
Finally, increased recombination losses also occur as the density of recombination centers increases with
crystal damage (see Sect. 15.2.3). Thus, in general, one must correct for the PHD in heavy ion spectroscopy.
The measured pulse height P and the energy E of the heavy charged particle is often related by

E = Sn + δ, (20.168)

16 Theactive zero time detector provides another method to determine the mass-energy relationship, albeit generally less accurate
[Sachs et al. 1966]
dE E
E = (E  + ΔE)ΔE = k1 M Z 2 ln  KM Z 2 . (20.167)
dx k2 M
Sec. 20.9. Charged-Particle Spectroscopy 1111



     







 
  

!  

!  

      

  

Figure 20.40. Pulse height dependence for channeled and non-channeled


40 Ar and 127 I ions along the [110] axis. Data are from Moak et al. [1966].

where S is a scaling constant and δ is the pulse height defect. For a common multichannel analyzer system,
S may be the equivalent energy per channel and n would be the channel number. Shown in Fig. 20.39 is a
comparison between the actual ion energies of various heavy ions and the associated pulse heights indicated
by channel number on a multichannel analyzer [Wilkins et al. 1971] and from which it is apparent that the
PHD increases with the Z number of the heavy ion.
It is notable that in at least one study the PHD seems to disappear with channeled ions [Moak et al.
1966]. The comparison was drawn between ions of two different masses, 40 Ar and 127 I. Much like sulphur
in Fig. 20.39, the PHD for Ar ions (with an atomic mass close to that of S) was small with little difference
between ions with or without channeling. However, there was clearly the appearance of a PHD for the
unchanneled iodine ions, which have a slightly larger atomic mass than that of silver, and the PHD for iodine
was similar to that of silver in Fig. 20.39. However, the PHD was similar to that of Ar when channeled, as
shown in Fig. 20.40. The reason for the difference is attributed to a lower stopping power −dE/dx of the
channeled ions and the reduction or absence of nuclear collisions. Further, the energy resolution reportedly
improved by a factor of three for the channeled ions. The experiment performed by Moak et al. [1966] seems
to confirm that it is nuclear collisions that are responsible for most of the PHD observed with heavy ions,
although the lower −dE/dx also reduces recombination losses. The observed energy resolution improvement
is probably because the variance term for non-ionizing energy losses becomes negligible for the channeled
ions. Attempts to correlate measured PHD to empirical formulas are in the literature (for example, Schmitt
et al. [1965]; Wilkins et al. [1971]). One general correlation offered by Schmitt et al. [1965] is based on the
assumption that two linear functions can be used to describe both the scaling constant and the PHD in
Eq. (20.168), namely
E = (a + a M )P + (b + b M ), (20.169)

where M  A is the mass (in u) of the ion and a, a , b, and b are experimentally determined constants
particular to the detector. The constants can be found by using a spectroscopic grade fission source, such
as 252 Cf. If PL denotes the 3/4-maximum in the pulse height for the lower mass (higher energy) peak
(PL = 0.75NL in Fig. 20.41) and PH denotes the 3/4-maximum in the higher mass (lower energy) peak
1112 Radiation Measurements and Spectroscopy Chap. 20

NL Lmax

Observed Counts (arbitrary units) NH Hmax 0.75NL


DL

0.75NH
DH DL
2
DH DL
2 DH 2
NV 2

0.1NL
DS

HS H L LS

Pulse Height (Channel Number)

Figure 20.41. Identifying parameters for a 252 Cf pulse


height spectrum. After Schmitt and Pleasonton [1966].

Table 20.3. Summary of SSB detector spectral metrics for Fig. 20.41.

252 Cf 235 U

Parameter Reasonable Expected Expected


Limit Value Value
NL /NV > 2.85 ∼ 2.9 ∼ 19
NH /NV ∼ 2.2 ∼ 2.2 ∼ 12.5
NL /NH − ∼ 1.3 1.49-1.55
ΔL/(L − H) < 0.38 ∼ 0.36 0.22-0.23
ΔH/(L − H)  0.45  0.44 0.35-0.36
(H − HS)/(L − H) < 0.70  0.69 0.38-0.39
(LS − L)/(L − H)  0.49  0.48 0.27-0.28
(LS − HS)/(L − H)  2.18 ∼ 2.17 ∼ 1.66

(PH = 0.75NH in Fig. 20.41) , the constants are found to be [Weissenberger et al. 1986]
a0 a0
a= , a = , b = b0 − aPL and b = b0 − a PL . (20.170)
PL − PH PL − PH
252
For a Cf source,17
a0 = 24.300, a0 = 0.0283, b0 = 90.397, and b0 = 0.1150, (20.171)
all in units of MeV.
17 These constants are slightly different from the original work by Schmitt et al. [1965]. Weissenberger et al. [1986] state the
prior values systematically overestimated the kinetic energies by 1-2%.
Problems 1113

For a 252 Cf source measured with an SSB detector, certain parameters can be used to provide quantitative
metrics for the particle detector [Schmitt and Pleasonton 1966] that are shown in Fig. 20.41. The vertical
axis, with labels N , refer to the number of observed counts at relative pulse heights (channel numbers).
These metrics include peak ratios, such as NL /NV , NH /NV , and NL /NH . Of these, Schmitt and Pleasonton
[1966] indicate that most important is the peak-to-valley ratio NL /NV with a reasonable lower limit of 2.85.
With NL /NV , the FWHM resolution for a 70-MeV ion (Br, for instance) should be approximately 1 MeV,
while that for a corresponding iodine ion is 1.4 MeV. Listed in Table 20.3 are other performance metrics.

PROBLEMS
1. Consider the design of an experiment to obtain the data in Example 20.1. The total interaction coefficient
μ of the absorbing foils contains a scattering component which, instead of absorbing photons traveling
from the point source to the detector, scatter some of the source photons. Some of these scattered
photons still reach the detector and are counted as uncollided or unattenuated photons. Design an
experiment, i.e., the size and placement of the foils with respect to the source and detector, that
minimizes the scattered component of photons that reach the detector.

2. Show that for small rtr Eq. (20.29) is approximately the same as Eq. (20.27).

3. Derive Eqs. (20.90).

4. Consider the count data in Table 20.4. (a) Write a program to find the best fit parameters of this
isolated peak. With the fit model of Eq. (20.71), use the linear least-squares method as in Example 20.2
and by trial and error find the peak centroid and standard deviation to obtain the best fit. (b) How
many counts are there under the peak?
Table 20.4. A portion of a spectrum around the 911.2-keV 228 Ac full-energy
peak in the background spectrum shown in Fig. 21.7.

Ei yi Ei yi Ei yi Ei yi
(keV) cnts (keV) cnts (keV) cnts (keV) cnts
0.9066 589 0.9088 601 0.9109 2349 0.9131 537
0.9069 625 0.9090 692 0.9112 1985 0.9134 568
0.9071 596 0.9093 878 0.9115 1467 0.9137 591
0.9074 582 0.9096 1039 0.9118 1148 0.9139 597
0.9077 590 0.9099 1511 0.9120 831 0.9142 586
0.9079 640 0.9101 1867 0.9123 721 0.9145 581
0.9082 624 0.9104 2287 0.9126 585 0.9148 606
0.9085 615 0.9107 2430 0.9128 590 0.9150 594

5. Use the non-linear least-squares method to fit simultaneously all the parameters of Eq. (20.71) to the
data in the above problem.

6. Derive Eq. (20.155).

7. Show that fitting Eq. (20.104) to NE , NF and NP the parameters in the quadratic fit are

α = (1/2)[NE + NF − 2NP ], β = (1/2)(NF − NE ) − nP (NF + NE − 2NP )


1114 Radiation Measurements and Spectroscopy Chap. 20

and
NE − NF NE + NF − 2NP
γ = N P + nP + n2P .
2 2
Then derive the expressions for the channel number and the maximum peak count given by Eqs. (20.105)
and (20.106).
8. Show that the skewness factors defined in Eq. (20.111) are unity for a Gaussian peak.
9. Determine the corrected peak channel and counts for the peak shown in Fig. 20.18, but shifted slightly
so that now CP = 10, 000 at channel 3365 and CE = 9910 and CF = 7748. The peak is still located
between channels NL = 3351 and nR = 3374.
10. In Tables 20.5 and 20.6 are the channels and counts observed for the 214 Bi 2204.1-keV and 40 K 1460.8-
keV full-energy peaks, respectively. Estimate the resolution in keV and % of the HPGe detector used
to obtain these data.
Table 20.5. A portion of a spectrum around the 2204.1-keV 214 Bi full-energy
peak in the background spectrum shown in Fig. 21.7.

yi yi yi yi
n n n n
cnts cnts cnts cnts
8073 71 8081 175 8089 682 8097 95
8074 82 8082 225 8090 609 8098 79
8075 74 8083 280 8091 543 8099 92
8076 81 8084 441 8092 390 8100 74
8077 88 8085 542 8093 332 8101 68
8078 70 8086 621 8094 207 8102 71
8079 102 8087 687 8095 157 8103 75
8080 155 8088 735 8096 138 8104 65

Table 20.6. A portion of a spectrum around the 1460.8-keV 40 K full energy


peak in the background spectrum show in Fig. 21.7.

yi yi yi yi
n n n n
cnts cnts cnts cnts
5343 362 5351 3871 5359 36336 5367 450
5344 360 5352 7064 5360 29415 5368 288
5345 351 5353 12202 5361 21395 5369 226
5346 381 5354 19092 5362 13901 5370 189
5347 509 5355 26669 5363 8260 5371 177
5348 672 5356 34041 5364 4260 5372 141
5349 1159 5357 38791 5365 1992 5373 175
5350 1996 5358 39769 5366 968 5374 157

11. Explain why the resolution of a gamma-ray spectrometer that uses a scintillator is usually expressed as
a percentage, while that of a semiconductor spectrometer is usually given in energy units.
12. Using the detector configuration of Fig. 20.20, derive the expression for Eq. (20.121).
13. With the result of Eq. (20.145) and the constraint that TA = tG + tB , derive an expression for the
optimum source count time tG in terms of the available time tA .
14. You have a total of 5 minutes each to conduct measurements of numerous radioactive activation samples,
including the background measurement and the gross measurement. Given that on average g  3500
References 1115

cm and the average background is b  100 cpm, find the optimized times for the gross and background
measurements.

15. You have a 300-nm-thick B4 C detector claimed to be a semiconductor neutron detector. The film was
grown with natural boron on n-type Si and has area 2 mm × 2 mm. Given a thermal neutron (2200 m
s−1 ) flux of 104 cm−2 s−1 , how long should a measurement be to discern with 98% confidence that it
really is a B4 C semiconductor detector and not a thin-film Si pn-junction detector? Hint: the thin-film
neutron detector expressions in Chapter 17 might be helpful.

16. Given the two different cylindrical NaI:Tl detector configurations in Fig. 20.42, find the detection effi-
ciency of coincidence events if the source is 22 Na for both configurations. Repeat for 60 Co.

7.5 cm
det 1
det 1 det 2 source
source
7.62 cm 7.5 cm

7.5 cm 10 cm
det 2
7.62 cm

(a) (b)
Figure 20.42. Coincidence counting geometry for two NaI:Tl de-
tectors.

17. Determine the critical angle required to prevent alpha particle channeling in a Si SSB detector with
surface direction 100.

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Chapter 21

Mitigation of Background in
Gamma-Ray Spectroscopy

Eventually, we reach ... the utmost limits of our [instruments]. There, we


measure shadows, and we search among ghostly errors of measurement
for landmarks that are scarcely more substantial.
Edwin Powell Hubble

Everything in the universe is constantly being irradiated by different types of directly or indirectly ionizing
radiation. On Earth we and our scientific instruments are bathed in radiation from many different sources.
In particular, radiation detectors respond in varying degrees to the different types of background radiation
incident on them (or even produced by them). Thus, any measurement of the radiation from a particular
source with any of the many detectors discussed in this book also contains responses from the ever present
background radiation field. The separation of the foreground response from the source under study from
the background response is a key element in radiation measurements. This separation generally becomes
increasingly difficult as the foreground component decreases in the combined responses and as the stochastic
nature of the detector response becomes more pronounced.
To increase the strength of the foreground component and to reduce stochastic fluctuations in the detector
measurement, several approaches can be used. Generally placing a detector close to a compact radiation
source that is being analyzed increases the response rate by way of the inverse square law while keeping
the background response rate relatively unchanged. Increasing the measurement time also generally reduces
statistical uncertainties in the output response provided that the radiation source does not vary appreciably
during the measurement time. The use of a detector with a larger sensitive volume, while increasing the
foreground response rate, also increases the background response rate; however, because of the larger number
of recorded events, statistical uncertainties are reduced. Often shielding structures are used to reduce
the amount of background radiation that reaches the detector. The use of detector shielding is especially
important to reduce the background in low-level counting applications involving weak sources. Finally, in
some cases multiple detectors with coincident and anti-coincidence circuitry can be used to reject signals
produced by background radiation.
To understand how background radiation affects the response of a detector, it is important to know how
the detector responds to different types of radiation (well covered in the preceding chapters), the sources
and strengths of background radiation, and how different materials and techniques can be used to shield a
detector from background radiation. Background radiation and methods to reduce its impact are the subject
of this chapter.

1119
1120 Mitigation of Background Chap. 21

21.1 Sources of Background Radiation


There are many sources of background radiation which can affect the response of a detector. These include (1)
cosmic rays incident on the earth’s atmosphere, (2) secondary particles produced by cosmic rays interacting in
the atmosphere, (3) naturally occurring radionuclides in materials near the detector, (4) naturally occurring
radionuclides in the detector itself, (5) radioactivity in the earth that produces terrestrial radiation and
in materials far from the detector, (6) radioactivity in the air surrounding the detector, and (7) man-made
radiation sources from particle accelerators, x-ray machines, and radionuclides from weapons tests or created
for medical or industrial use.

21.1.1 Cosmic Radiation


The earth is bombarded continuously by radiation originating from our sun, from sources within our galaxy,
and from sources far beyond our galaxy. The radiation as it reaches the earth’s atmosphere consists of 99%
of high-energy atomic nuclei and 1% electrons. Cosmic rays also contain some photons but with energies far
below those of the atomic nuclei. The highest observed photon energy is about 1014 eV, while the highest
energy for a fermionic cosmic ray is an astounding 3 × 1020 eV. The origins of the extra galactic cosmic rays
is still somewhat mysterious, but recent satellite observations suggest the supernova explosions and active
galactic centers produce some of this radiation.
Hydrogen nuclei (protons) constitute the major material component (90%) of cosmic rays, along with
alpha particles (9%) and some heavier atoms, decreasing in importance with increasing atomic number.
Cascades of nuclear interactions in the atmosphere, initiated by primary cosmic rays, give rise to many
types of secondary particles such as neutrons, kaons and pions. The kaons almost all decay to muons before
reaching the surface of the earth.1 The fluxes (in units of cm−2 s−1 MeV−1 ) of the various cosmic rays at
the earth’s surface are shown in Fig. 21.1. The primary and secondary cosmic rays also interact in the soil
(or water) and produce yet more photons and neutrons. The neutron flux is affected mostly by the water
content or the soil as is shown in Fig. 21.2. Below 1 MeV the secondary atmospheric produced neutrons
begin to slow down as they are moderated by the soil and air producing a characteristic 1/E slowing down
spectrum that at thermal energies assumes Maxwellian shape. The data for Fig. 21.1 and Fig. 21.2 were
generated by the freely downloadable program EXPACS [2018] which is based on the work of Sato et al.
[2006, 2008]. With this program the cosmic ray components can be determined at any altitude, location,
and at any time in the solar cycle.
As can be seen in Fig. 21.1, the intensity of cosmic rays reaching the surface of the earth is anti-correlated
with the solar activity, i.e., when the sun is most active in its 22-year cycle the cosmic ray intensity is the
lowest and, when the sun is least active, the cosmic ray intensity is at its highest. This counterintuitive anti-
correlation is a result of changes in the solar magnetic field. When the sun spot activity is at its greatest,
the solar magnetic field is at its strongest and deflects more cosmic rays away from the inner solar system.
Likewise, when the sun is least active, its magnetic field is weakest and allows more cosmic rays to reach
earth. Although this effect appears small on the logarithmic scale of Fig. 21.1, the intensity swing is about
50% for neutrons and 30% for photons at an energy of 1 MeV.

1 Muons μ+ and antimuons μ− are radioactive elementary particles with a rest mass energy equivalent of 105.7 MeV and a
mean lifetime of 2.197 μs. They decay as

μ− → e− + ν e + νμ or μ+ → e+ + νe + ν μ .

They interact with electrons, but lose little energy per interaction, and produce little bremsstrahlung. Consequently, they are
very penetrating. For example, a 1-MeV muon has a CSDA range of 470 cm in water, while a 1000-MeV muon has a 2426-m
range [Bevelacqua 2008].
Sec. 21.1. Sources of Background Radiation 1121

Figure 21.1. Ground-level fluxes of the various components of cos-


mic rays at the minimum (solid lines) and at the maximum of the
solar cycle (dotted lines). The ground is at average elevation of the
U.S. (2493 ft). Data generated by EXPACS [2018].

Figure 21.2. The neutron flux produced by cosmic radiation at ground-level for two
extreme volume fractions of water in the ground. Data generated by EXPACS [2018].
1122 Mitigation of Background Chap. 21

Figure 21.3. Anisotropy of gamma rays, neutrons, electrons and positrons produced by
cosmic radiation at ground-level. Plotted is the ratio R = 4πφ(E, θ)/φ(E) versus cosine
of the zenith angle. For an isotropic flux R = 1. The direction cos(θ) = 1 is the vertically
downward direction. The 4π integrated flux is shown in Fig. 21.1. Data were obtained
from EXPACS [2018].

The angular distribution of cosmic radiation that reaches the earth’s surface depends on the radia-
tion particle since the earth’s surface can affect, especially at lower energies, the reflection of the radia-
tion into the atmosphere. For example, muons are negligibly reflected and their angular flux φ(E, θ) ≡
d2 φ(E, θ)/{dE dΩ(θ)} cm−2 s−1 MeV−1 sr−1 is essentially zero in the upward directions, i.e., for nadir an-
gles θ > π/2. By contrast, neutrons at energies below about 0.1 MeV are almost isotropically distributed as
can be seen in Fig. 21.3. In the figure the ratio R ≡ 4πφ(E)/φ(E, cos(θ)) is plotted versus the cosine of the
nadir angle. Here cos θ = 1 refers to the directly downward direction. If the angular flux is isotropic R = 1.
As can be seen from Fig. 21.3 the angular flux becomes increasingly anisotropic in the downward direction.
Both as a useful measure and as a single cosmic-ray metric, the effective dose equivalent is widely used
to describe the intensity of cosmic rays. At earth’s surface, cosmic radiation dose rates are largely due
to muons and electrons. The intensity and angular distribution of galactic radiation reaching the earth
is affected by the earth’s magnetic field and perturbed by magnetic disturbances generated by solar flare
activity. Consequently, at any given location, cosmic ray doses may vary in time by a factor of 3. At any
given time, cosmic ray dose rates at sea level may vary with geomagnetic latitude by as much as a factor of
8, being greatest at the pole and least at the equator. The global average cosmic ray dose equivalent rate at
sea level is about 240 μSv per year for the directly ionizing component and 20 μSv per year for the neutron
Sec. 21.1. Sources of Background Radiation 1123

component [UN 1988]. Cosmic ray dose rates also increase with altitude. At geomagnetic latitude 55o N,
for example, the absorbed dose rate in tissue approximately doubles with each 2.75 km (9000 ft) increase in
altitude, up to 10 km (33,000 ft). The neutron component of the dose equivalent rate increases more rapidly
with altitude than does the directly ionizing component and dominates at altitudes above about 6 km [UN
1988].
Solar cosmic rays associated with flares are mainly hydrogen and helium nuclei. While of too low an
energy to contribute to radiation doses at the surface of the earth, solar-flare radiation, which fluctuates
cyclically with an 11-year period (from to minimum to minimum sun spot activity), perturbs earth’s magnetic
field and thereby modulates galactic cosmic-ray dose rates with the same period. As the sun becomes more
active, the solar wind from the sun increases and deflects more of the cosmic radiation from reaching earth.
This decrease in cosmic ray activity at ground level with increasing solar activity is seen in Fig. 21.1 where
the dotted lines are ground-level fluxes at maximum solar activity which are seen to be slightly lower than
the solid lines at the solar minimum. Thus, maxima in solar flare activity lead to minima in dose rates.
Solar flare radiation, in comparison to galactic cosmic rays, is of little significance as a hazard in aircraft
flight or low orbital space travel. On the other hand, solar-flare radiation presents a considerable hazard to
personnel and equipment in space travel outside the earth’s magnetic field.
Released continuously from the sun, as an extension of the corona, is the solar wind, a plasma of low-
energy protons and, presumably, very low-energy electrons. The solar wind does not present a radiation
hazard, even in interplanetary space travel. However, it does affect the interplanetary magnetic field and the
shape of the geomagnetically trapped radiation belts. These radiation belts are thought to be supplied by
captured solar-wind particles and by decay into protons and electrons of neutrons created by interactions of
galactic cosmic rays in the atmosphere. The trapped radiation can present a significant hazard to personnel
and equipment in space missions.
Galactic Cosmic Rays
Cumulative energy spectra for the various components of the
galactic cosmic radiation incident on the earth’s atmosphere are
illustrated in Fig. 21.4. These spectra may be approximated as

A
φ(E > Eo )  , (21.1)
(Mo c2 + Eo )n

in which φ(E > Eo ) is the flux density of particles with energies


greater than Eo , Mo c2 is the rest-mass energy equivalent of the
particles, A and n are parameters which, generally, depend on
the state of the solar cycle.
As a result of nuclear spallation reactions with constituents of
the atmosphere, secondary neutrons, protons, and pions, mainly,
are produced. Subsequent pion decay results in electrons, pho-
tons, neutrons, and muons. Muon decay, in turn, leads to
secondary electrons, as do Coulombic scattering interactions of
charged particles in the atmosphere.
Figure 21.4. Integral energy spectra (i.e., the
Except for short-term influences of solar activity, galactic cos- flux of particles with energies > E) for var-
mic radiation has been constant in intensity for at least several ious components of the galactic cosmic radia-
thousand years. The influence of solar activity is cyclical. The tion. Light nuclei, 3 ≤ Z ≤ 5, medium nuclei
principal variation is on an 11-year cycle, but there are very 6 ≤ Z ≤ 9, and heavy nuclei Z ≥ 10. Solid
lines are for the solar minimum and dashed lines
small diurnal variations and evidence of a 22-year cycle as well are for the solar maximum. Data from Haffner
as 27-day quasi-periodic variations [Haffner 1967]. [1967].
1124 Mitigation of Background Chap. 21

The geomagnetic field of the earth is responsible for limiting the number of cosmic rays which can
reach the atmosphere. For particles of atomic number Z vertically incident at geomagnetic latitude λ, the
minimum momentum for a cosmic ray to reach the atmosphere is proportional to Z cos4 λ [Haffner 1967].
This dependence accounts for a strong effect of latitude on cosmic-ray dose rates.

Solar Flare Particulate Radiation


Solar flare particles are mostly protons and alpha particles, predominantly the former. Electrons are thought
to be emitted as well, but with energies less than those of protons by a factor equal to the ratio of the rest
masses. These flares can disrupt earth’s ionosphere which affects long-range radio communications. They
have little effect at the earth’s surface and produce little change in the background experienced by radiation
detectors. However, solar flares can be accompanied by coronal mass ejections (CME) which can cause large
geomagnetic storms that, in turn, can disable satellites and shut down electrical grids for hours. For space
missions outside the atmosphere, solar flares must be considered in order to protect both astronauts and
their equipment.
Energy spectra are highly variable, as are temporal
Table 21.1. Measured fluences (cm−2 ) outside earth’s variations of intensity. Haffner [1967] describes records
atmosphere produced by the solar flare that occurred July
10, 1959. Source: Haffner [1967]. of solar flares during the 1956-1961 interval which en-
compasses the 1959 maximum in activity. The large
protons alpha particles
event of 10 July, 1959, for example, resulted in the flu-
E > 10 MeV 4.5 × 109 E > 40 MeV 1.6 × 108 ences (cm−2 ) outside the earth’s atmosphere given in
E > 30 MeV 1.0 × 109 E > 120 MeV 2.4 × 107
Table 21.1. A typical course of events for a flare is as
E > 100 MeV 1.4 × 108 E > 400 MeV 5.0 × 105
follows. Gamma and x-ray emission takes place over
about 4 hours as is evidenced by radio interference. The first significant quantities of protons reach the earth
after about 15 hours and peak proton intensity occurs at about 40 hours after the solar eruption [NCRP
1989].

21.1.2 Natural Occurring Radioactivity


Cosmogenic Radionuclides
Cosmic-ray interactions with constituents of the atmo- Table 21.2. Global distribution of cosmogenic radionu-
sphere, sea, or earth, but mostly with the atmosphere, clides produced in the atmosphere.
lead directly to radioactive products. Capture of sec- 3H 7 Be 14 C 22 Na
ondary neutrons produced in primary interactions of cos-
Global Inventory (PBq) 1300 37 8500 0.4
mic rays leads to the formation of many more radionu-
Distribution (%)
clides. However, the thermal-neutron flux at sea level stratosphere 6.8 60 0.3 25
is only about 8 cm−2 h−1 [Morgan 1967] and the to- troposphere 0.4 11 1.6 1.7
−2 −1
tal neutron flux density is only about 30 cm h [UN land surface/biosphere 27 8 4 21
1988]. Thus, neutron capture in the earth’s crust or the mixed ocean layer 35 20 2.2 44
sea is of little importance in comparison with capture in deep ocean 30 0.2 92 8
36 ocean sediments 0.4
the atmosphere, except for production of long-lived Cl
Source: UN [1982].
[NCRP 1975]. Of the nuclides produced in the atmo-
3 7 14 22
sphere, only H, Be, C, and Na contribute appreciably to human radiation exposure. The distribution
of these cosmogenic radionuclides is shown in Table 21.2. Radionuclides borne by the 107 kg of “space
dust” reaching the earth annually have a total specific activity of less than 450 pCi kg−1 and result in only
extremely low atmospheric concentrations [NCRP 1975].
Over the past century, combustion of fossil fuels and the emission of CO2 not containing 14 C has diluted
the cosmogenic content of 14 C in the environment. Moreover, since World War II, artificial introduction of
Sec. 21.1. Sources of Background Radiation 1125

3
H, 14 C, and other radionuclides,2 into the environment by human activity has been significant, especially
as a result of atmospheric nuclear-weapons tests. Consequently, these nuclides no longer exist in natural
equilibria in the environment.
Tritium is produced in the atmosphere mainly from the 14 N(n,t)12 C and the 16 O(n,t)14 N reactions. It has
a half-life of 12.3 years and, upon decay, releases one beta particle with maximum energy 18.6 keV (average
energy 5.7 keV). Tritium exists in nature almost exclusively as HTO but may be partially incorporated into
organic compounds such as those in wood, a common construction material. In continental surface waters
the ratio of 3 H to stable hydrogen is 3.3 × 10−18 (corresponding to 0.00039 Bq cm−3 ). Because 3 H emits
only a low-energy beta particle, it is generally of little concern in most low-level counting applications. Only
if a liquid scintillator is used to look for tritium leaks from nuclear facilities that also produce tritium does
the incorporation of cosmogenic tritium in the scintillator become a concern.
The nuclide 14 C is produced mainly from the 14 N(n,p)14 C reaction. It exists in the atmosphere as CO2 ,
but the main reservoir is the ocean. It has a half-life of 5730 years and decays by beta particle emission,
each decay resulting in an electron of maximum energy 157 keV (average energy 49.5 keV). The natural
atomic ratio of 14 C to stable carbon is 1.2 × 10−12 (corresponding to 0.226 Bq 14 C per gram of carbon)
[NCRP 1975]. Because 14 C emits only beta particles, it contributes negligibly to the photon background
save low-energy bremsstrahlung photons below 157 keV. Only in low-energy beta counting measurements is
it of concern.
The 7 Be radionuclide, with a half-life of 53.4 days, is also produced by cosmic ray interactions with
nitrogen and oxygen in the atmosphere. It decays by electron capture, 10.4 percent of the captures resulting
in the emission of a 478-keV gamma ray. Environmental concentrations in temperate regions are about 3000
Bq m−3 in surface air and 700 Bq m−3 in rainwater [UN 1982]. A background gamma-ray spectrum often
shows a very small 478-keV full energy peak.
The radionuclide 22 Na is produced in spallation interactions of atmospheric argon with high-energy
cosmic-ray secondary neutrons. It has a half-life of 2.602 y, decaying by positron emission (90 percent)
and electron capture (10 percent). The positron has a maximum energy of 546 keV (average energy 216
keV). Essentially all decays are accompanied by emission of a 1.275-MeV gamma ray from the excited 22 Ne
daughter. Although the 1.275-MeV gamma ray may be observed in a background spectrum taken by a very
sensitive gamma-ray spectrometer, the 0.511-MeV positron annihilation photon which usually is present in
a background spectrum is attributable mostly to cosmic-ray positrons.
Activation by Cosmic Ray Neutrons
The neutrons produced by spallation reactions in the atmosphere and ground by cosmic rays can lead to
the buildup of radionuclides in materials stored at ground level. Although of little radiological concern,
these radionuclides can contribute to the background spectrum in underground ultra-low-level facilities. For
example, pre-World War II steel, i.e., steel without any fission products, was tried as a shield against the
gamma rays emitted from lead shielding but found to be too contaminated by 54 Mn (T1/2 = 312.1 d) that
was produced by cosmic ray neutrons interacting with 54 Fe when the old steel was stored for years at ground
level [Brodzinski et al. 1985]. Thus, steel should not be used in such ultra-low-level facilities unless it has
been stored underground for many years. However, for less sensitive facilities, activation of steel is usually
of little concern.
One other example is the use of copper, which is used in spectrometer facilities for both shielding and
detector electronics. Electrolytic copper, while expensive, generally has very low impurity levels from the

2 One such nuclide is 137 Cs (T1/2 = 30.0 y) which, upon decay, emits a 661.7-keV gamma ray, which is found in most background
gamma-ray spectra. The presence of this radionuclide in a sample measured in a low-level counting chamber indicates the
sample dates from the post 1950 era and is used, for example, to determine if a purportedly old wine (or its bottle) is truly
made of pre-1950 material.
1126 Mitigation of Background Chap. 21

naturally occurring radionuclides. However, storage at ground level allows the buildup of 60 Co from energetic
cosmic ray neutrons through the 63 Cu(n,α)60 Co reaction. So copper for use in ultra-low-level counting
facilities must be moved underground as soon as possible after its purification.
Primordial Radionuclides
Of the many radioactive species present when the earth formed 4 billion years ago, some 17 extremely long-
lived radionuclides still exist as singly occurring or isolated radionuclides, i.e., as radionuclides not belonging
to a decay chain. These terrigenous (primordial) radionuclides are listed in Table 5.1. Of these primordial
radionuclides, only 40 K contributes significantly to the gamma-ray background.
The radionuclide 40 K is a major contributor to human exposure from natural radiation. Present in an
isotopic abundance of 0.0118 percent, it has a half-life of 1.227 × 109 y, decaying both by electron capture
(11 percent) and beta-particle emission (89 percent). The beta particle has a maximum energy of 1312 keV
(average energy 509 keV). Electron capture results in emission of a 1461-keV gamma ray in 10.7 percent
of decays. Very low energy Auger electrons and x rays are also released from electron capture (Kocher
1981). The average elemental concentrations of potassium in Reference Man3 is 2 percent. Annual doses in
Reference Man are 140 μGy to bone surface, 170 μGy on average to soft tissue, and 270 μGy to red marrow
(UN 1982). 40 K also contributes in a major way to external exposure. The average specific activity of the
nuclide in soil, 12 pCi g−1 (0.44 Bq g−1 ), results in an annual whole-body dose equivalent of 120 μSv (12
mrem) [UN 1982]. However, actual specific activities can vary considerably depending on the type of soil as
is shown later in Table 21.5.
Decay Series of Primordial Origin
Each naturally occurring radioactive nuclide with Z > 83 is a member of one of three long decay chains,
or radioactive series, stretching through the upper part of the Chart of the Nuclides. These radionuclides
decay by α or β − emission and they have the property that the number of nucleons (mass number) A for
each member of a given decay series can be expressed as 4n + i, where n is an integer and i is a constant (0,
2, or 3) for each series. The three naturally occurring series are named the thorium (4n), uranium (4n + 2),
and actinium (4n + 3) series, named after the radionuclide at, or near, the head of the series.
Two of these primordial decay series, identified by the long-lived parents 238 U and 232 Th contribute
appreciably to the natural gamma-ray background. Another series headed by the primordial 235 U radionu-
clide contributes very little to the radiation background and makes a negligible contribution to the radiation
background.4
The three naturally occurring series are shown schematically in Figs. 21.5 and 21.6, and the principal
radiations emitted by members of the two important series are given in Tables 21.3 and 21.4. Within
each series are subseries headed by a radionuclide with a half-life much greater than those of its daughters.
Although all the members of a series are not likely to be in radioactive secular equilibrium in nature because
of chemical or physical reasons, members of a subseries are more likely to be so. The subseries headed by
the gases 220 Rn and 222 Rn are of special importance and are treated separately in a subsequent section.
The radiations emitted by members of the primordial decay chains and listed in Tables 21.3 and 21.4 are
but a small fraction of all the radiations emitted. Most have frequencies less than the 0.5% cutoff used in

3 The Reference Man is a hypothetical person with the anatomical and physiological characteristics of an average individual
and is widely used in calculations that assess internal doses to various organs from various radiation sources. Specifically, he
is 20-30 years of age, weighs 70 kg, is 170 cm in height, and lives in a climate with an average temperature of 10◦ to 20◦ C
[ICRP 1975].
4 There is no naturally occurring series represented by 4n+1. This series was recreated after 241 Pu was made in nuclear reactors.
94
This series does not occur naturally since the half-life of the longest lived member of the series, 237 6
93 Np, is only 2.14 × 10 y,
much shorter than the lifetime of the earth. Hence, any members of this series that were in the original material of the solar
system have long since decayed away.
Sec. 21.1. Sources of Background Radiation 1127

234 238
92 U 92 U
245 ky 4.47 Gy
JJ
]
234m
91 Pa
1.17 m

? JJ
] ?
230 234
90 Th 90 Th
77 ky 24.1 d

?
226
88 Ra
1600 y

?
222
86 Rn
3.82 d

?
210 214 218
84 Po 84 Po 84 Po
138.4 d 164 μs 3.05 m
JJ
] JJ
]
210 214
83 Bi 83 Bi
5.013 d 19.9 m

? JJ
] ? JJ
] ?
206 210 214
82 Pb 82 Pb 82 Pb
stable 22.3 y 26.8 m

Figure 21.5. The 238 92 U (4n + 2) natural decay series. Alpha decay is depicted by downward
arrows and β − decay by arrows upward and to the left. Not shown are (1) the isomeric transition
to 234
91 Pa (0.16%) followed by beta decay to
234 U, (2) beta decay of 218 Po to 218 At (0.020%)

followed by alpha decay to 214 Bi, (3) alpha decay of 214 Bi to 210 Tl (0.0210%) followed by beta
decay to 210 Pb, and (4) alpha decay of 210 Bi to 206 Tl (0.000132%) followed by beta decay to
206 Pb. From Shultis and Faw [2017].
1128 Mitigation of Background Chap. 21

235
92 U
.704 Gy

231
91 Pa
32.8 ky
228
90 Th
232
90 Th JJ
] ?
227 231
1.913 y 14.05 Gy 90 Th 90 Th
JJ
] 18.7 d
98.6%
1.06 d
228
89 Ac JJ
] ?
227
6.13 h 89 Ac

? JJ
] ? 21.8 y
224 228
88 Ra 88 Ra ?
223
3.63 d 5.75 y 88 Ra 1.38%

? 11.4 d
220
86 Rn JJ
] ?
223
55.61 s 87 Fr

? 21.8 m
212 216
84 Po 84 Po ?
219
0.298 μs 0.146 s 86 Rn
JJ64.1%
] 3.96 s
212
83 Bi
60.55 m

? JJ
] ?
208 212
82 Pb 82 Pb ?
35.9%
211 215
stable 10.64 h 84 Po 84 Po
JJ
] ? 0.52 s
0.28%
1.78 ms
208
81 Tl JJ
]
211
3.053 m 83 Bi
2.14 m

? JJ
] ?
207 211
82 Pb 99.7% 82 Pb
stable 36.1 m
JJ
] ?
207
81 Tl
4.77 m

Figure 21.6. The 232 235


90 Th (4n) natural decay series (left) and the 92 U (4n + 3) natural decay
series (right). Alpha decay is depicted by downward arrows and β − decay by arrows upward and
to the left. Not shown in the 235
92 U series on the right are two very minor side chains: (1) alpha
decay of 223 Fr (0.004%) to 85 At which beta decays to 223 Ra (3%) or alpha decays to 215 Bi which
beta decays to 215 Po, and (2) the beta decay of 215 At (< 0.001%) followed by alpha decay to
211 Bi. From Shultis and Faw [2017].
Sec. 21.1. Sources of Background Radiation 1129

Table 21.3. Principal radiations from nuclides in the 232 Th decay series. Not
listed are x rays, conversion and Auger electrons, and beta or gamma rays with
frequencies less than 0.5%.
Alpha particles Beta particles Gamma rays
Eα freq. Emax Eav freq. Eγ freq.
Nuclide
(keV) (%) (keV) (keV) (%) (keV) (%)
232
Th 3811.1 0.069 12.3 7.1
3947.1 21.7
4012.3 78.2
228
Ra 39.5 7.24 100
228
Ac 410 117.50 1.76 99.51 1.26
446 129.00 2.43 129.07 2.42
451 130.82 1.12 153.98 0.72
488 142.79 4.19 209.25 3.89
491 143.73 3.0 214.85 0.76
496 145.32 1.15 270.25 3.46
603 181.0 7.6 328.00 2.95
684 208.9 0.60 338.32 11.27
702 215.3 1.2 409.46 1.92
907 288.8 0.67 463.00 4.40
966 310.2 3.11 562.50 0.87
981 315.7 5.8 674.75 2.10
1011 327.0 5.90 726.86 0.62
1111 364.7 3.11 755.32 1.00
1165 385.0 29.9 772.29 1.49
1806 609.3 0.59 794.95 4.25
1738 609.7 11.65 830.49 0.54
2076 747.0 7 835.71 1.61
904.20 0.77
911.20 25.8
964.77 4.99
968.97 15.8
1247.08 0.50
1459.14 0.83
1588.20 3.22
1630.63 1.51
228
Th 5340.3 26.0 84.37 1.19
5423.2 72.7
224
Ra 5448.6 5.06 240.0 4.10
5685.4 94.92
220
Rn 6288.1 99.90
216
Po 6779 99.89
212
Pb 154.6 41.1 5.08 115.2 0.60
331.3 93.5 83.1 238.6 43.6
569.9 171.7 11.9 300.1 3.30
212
Bi 6010 5.0 39.86 1.06
6300 26.0
6340 35.0
212
Po 8784.9 100.
208
Tl 1038.1 342.9 3.18 252.6 0.78
1079.2 358.7 0.63 277.4 6.8
1290.6 441.5 24.2 510.8 22.6
1523.9 535.4 22.2 583.2 85.0
1801.3 649.5 49.1 763.1 1.79
860.6 12.5
2614.5 99.7
Source: NuDat [2017].
1130 Mitigation of Background Chap. 21

Table 21.4. Principal radiations from nuclides in the 238 U decay series. Not
listed are x rays, conversion and Auger electrons, and beta or gamma rays with
frequencies less than 0.5%.
Alpha particles Beta particles Gamma rays
Eα freq. Emax Eav freq. Eγ freq.
Nuclide
(keV) (%) (keV) (keV) (%) (keV) (%)
238
U 4147 23
4196 77
234
Th 86 22.3 1.5 63.29 3.7
106 27.7 6.4 92.38 2.13
107 27.8 14.0 92.80 2.10
199 53.9 78.0
234m
Pa 1224 405.6 1.00 1001.0 0.842
1459 496.0 0.95
2269 820.5 97.57
234
U 4722.4 28.42
4774.6 71.38
230
Th 4620.5 23.40
4687.0 76.3
226
Ra 4601 6.61 186.2 3.64
4784.3 93.84
222
Rn 5489.5 99.92
218
Po 6002.4 99.98
214
Pb 180 48.3 2.75 53.23 1.08
485 143.1 1.04 241.99 7.25
667 205.5 45.9 258.86 0.531
724 225.6 40.2 295.22 18.42
1019 334.9 11.0 351.93 35.60
785.96 1.06
839.07 0.583
214
Bi 788 248.2 1.244 609.32 45.49
822 260.9 2.78 665.45 1.531
977 318.2 0.557 768.36 4.89
1066 352.1 5.60 806.18 1.264
1077 356.5 0.855 934.06 3.107
1151 385.1 4.345 1120.29 14.92
1253 424.6 2.450 1155.21 1.633
1259 427.1 1.431 1238.12 5.834
1275 433.5 1.177 1280.98 1.434
1380 474.9 1.588 1377.67 3.988
1423 492.0 8.14 1385.31 0.793
1505 525.3 16.96 1401.51 1.330
1540 539.4 17.57 1407.99 2.394
1609 567.2 0.61 1509.21 2.130
1727 615.4 3.12 1583.20 0.705
1855 668.1 0.89 1661.27 1.047
1892 683.7 7.35 1729.60 2.878
2661 1007.5 0.58 1764.49 15.30
3270 1268.8 19.10 1847.43 2.025
2118.51 1.160
2204.06 4.924
2447.70 1.548
214
Po 7686.8 99.989
210
Pb 17.0 4.16 84 46.5 4.05
63.5 16.16 16
210
Bi 1162.2 389.0 100.0 265.6 51.0
304.6 28.0
329.6 0.66
344.3 0.71
368.9 0.66
210
Po 5304.3 100.0
Source: NuDat [2017].
Sec. 21.1. Sources of Background Radiation 1131

these tables. For example 228 Ac emits a known 54 different beta particles and an astounding 246 different
energy gamma rays! The background energy spectrum, thus, is almost a continuum of different energy
particles emitted by the decay chain radionuclides, of which only a few occur sufficiently frequently that
their contribution to the gamma-ray spectrum is identifiable.

Radionuclide Concentrations in Different Materials


Primordial radionuclides and their radioactive daughters are present in all natural materials. Such radioactive
material is classified as NORM (Naturally Occurring Radioactive Material). The concentrations of these
radionuclides is often altered by extraction, manufacturing, and processing of the natural materials. These
materials with altered radionuclide concentrations are sometimes classified as TENORM (Technologically
Enhanced Normal Radioactive Material). For regulatory purposes some man-made radioactivity such as
fallout from nuclear weapons tests, is also considered part of the natural background.

Table 21.5. Typical naturally occurring radionuclide concentrations in U.S. rocks


and soils.
Average specific activity (Bq kg−1 )
Rock/soil absorbed dose rate
40 K 238 U 232 Th in air (nGy h−1 )

Igneous Rock
acidic 100 60 80 120
intermediate 70 23 32 62
mafic 240 11 11 23
ultrabasic 150 0.4 25 23
Sedimentary Rock
limestone 90 2.8 7 20
carbonate – 2.7 8 17
sandstone 370 20 8 32
shale 700 45 45 79
Soil Type
serozem 650 30 50 74
gray-brown 700 28 40 69
chestnut 550 25 37 60
chernozem 400 20 36 51
gray forest 370 18 27 41
sodpodzolic 300 15 22 34
podzolic 150 9 12 19
boggy 90 6 6 11
world average 370 25 25 46
Coal
United States 50 20 22

Source: UN [1977].

Typical natural radionuclide activity concentrations in several soils and rocks are listed in Table 21.5.
Also listed are dose rates in air 1 m above the nuclide-bearing material, calculated on the basis of radioactive
equilibrium throughout the entire series. These dose rates are seen to be quite comparable to the back-
ground dose rate of 88 nGy/h to which the average person in the U.S. is exposed from external terrestrial
radionuclides.
1132 Mitigation of Background Chap. 21

21.1.3 Airborne Radioactivity


Sources of radiation are also present in the air. Dust from soil or construction activities can lead to airborne
naturally occurring radionuclides. However, a constant source of airborne radioactivity is from radon and its
daughters. Decay of radon and its daughters in the atmosphere leads first to individual unattached ions or
neutral atoms. The ions or atoms may become attached to aerosol particles, the attachment rate depending
in a complex manner on the size distribution of the particles. Radioactive decay of an attached ion or atom,
because of recoil, usually results in an unattached daughter ion or atom. Either attached or unattached
species may be deposited (plate out) on surfaces, especially in indoor spaces, the rate depending on the
surface-to-volume ratio of the space. Because of plate out, radon daughter products in the atmosphere are
not likely to be in equilibrium with the parent.
222
Rn and its daughters ordinarily present a greater radiological hazard than 220 Rn (thoron) and its
daughters, largely because the much shorter half-life of 220 Rn makes decay more likely prior to release
into the atmosphere. Relatively little is known about the rates of release, diffusion, inhalation, plate-out,
attachment, etc. for 220 Rn and its daughters, and most studies have emphasized the more important 222 Rn
series shown below.
α α β− β− α
222
86 Rn −→ 218
84 Po −→ 214
82 Pb −→ 214
83 Bi −→ 214
84 Po −→ 210
82 Pb (22.2 y). (21.2)
3.82 d 3.05 m 26.8 m 19.9 m 164μs

Airborne decay products beyond 214 Po are of little consequence since 210 Pb has such a long half-life that it
becomes bound to surfaces before it decays.
The alpha particles emitted by these airborne radionuclides are of little concern in most radiation measure-
ments except in the case of alpha-particle spectrometers for which they contribute to the energy spectrum.
The alpha particles from radon daughters are also of radiological concern because they can become lodged
in the pulmonary-bronchial system and produce large doses to the epithelial lung tissues [Faw and Shultis
1999]. Of greater concern from a radiation measurement perspective are the gamma rays emitted by 214 Pb
and 214 Bi (see Table 21.4). These gamma rays are prominent in most gamma-ray background spectra.
Outdoor Radon Activity
The noble gas radon diffuses into the atmosphere from rocks, soils, and building materials containing pro-
genitor radionuclides. The exhalation rate of 222 Rn from rocks and soils is highly variable, ranging from 0.2
to 70 mBq m−2 s−1 . An area-weighted average for continental areas, exclusive of Antarctica and Greenland,
is 16 mBq m−2 s−1 [UN 1988]. Exhalation from the surface of the sea is only about 1% of that from land
areas. Rain, snow, and freezing decrease exhalation rates so that they are generally lower in winter than in
summer. Barometric pressure and wind speed also affect exhalation rates, decreasing pressure or increasing
wind speed causing the rate to increase.
Radon and daughter products are dispersed in the atmosphere by turbulent diffusion and convection.
Extreme conditions of atmospheric stability can lead to ground-level concentrations differing by as much as
a factor of 100. Associated with conditions of atmospheric stability are marked diurnal variations in ground-
level concentrations, with minima at noon and maxima at midnight being associated respectively with greater
and lesser atmospheric instability. Concentrations decrease with altitude, with those of 220 Rn decreasing
more rapidly because of the shorter half-life of the parent. In the absence of precipitation, parent-daughter
equilibrium is approached at elevations exceeding about 100 m. However, rainfall may remove daughter
products from the atmosphere, causing absorbed dose rates in air at ground level to be as much as twice
normal.
Mean annual concentrations of 222 Rn above continental areas range from 1 to 10 Bq m−3 , with 5 Bq
−3
m and an equilibrium factor of 0.8 being typical (UN 1988). Typical mean annual concentrations over the
ocean and over island areas are 0.1 Bq m−3 . Concentrations of 220 Rn daughters are typically 10% of those
Sec. 21.2. Mitigation of the Radiation Background 1133

of 222 Rn daughters. Anomalously high levels often exist near coal-fired and geothermal power stations and
near uranium-mine tailings.
Indoor Radon Activity
Most spectroscopy is performed inside some structure or in rooms that are located at or below ground level
where concentrations of radon and its daughters can build up to levels several times those outdoors. Because
of the short lifetimes of the daughters, the members of the radon decay chain ideally would be in secular
equilibrium, i.e., the activity concentration of the daughters Ci would equal that of 222 Ra Co . However,
because of plate-out and settling, members of the decay chain are seldom in equilibrium. An equilibrium
factor fi , defined as fi = Ci /Co , typically has values around 0.5.
Indoor radon sources include exhalation from soil, building materials, water, ventilation air, and natural
gas if unvented (as used in cooking). Exhalation from soil can be a significant contribution if a building
has cracks or other penetrations in the basement structure or if the building has unpaved and unventilated
crawl spaces. Water usage in buildings can present a significant source of Rn if concentrations in the water
exceed about 10 kBq m−3 . In the United States, concentrations of 222 Rn in natural gas average 0.7 kBq
m−3 but in some states the average is as high as 2 kBq m−3 . Radon precursor concentrations in building
materials are highly variable. Greater concentrations occur in phosphogypsum and in concrete based on fly
ash or alum shale. Sealing concrete surfaces with materials such as epoxy-resin paints greatly reduces radon
exhalation. Indoor airborne radon and daughter concentrations depend not only on exhalation of the parent
gas from surfaces, but also on intake and loss of radionuclides through ventilation and plate-out of daughters
on interior surfaces. The rate of plate-out depends on the unattached fraction which is influenced greatly by
humidity and by the presence of aerosols (smoke, dust, etc.).

21.1.4 Modern Radiation Sources


In our modern technological world, new sources of ionizing radiation have been introduced. Radioisotopes
made by humans are used in many applications in medicine and industry. Likewise machines that produce
penetrating radiation are now widely used. For example, electron accelerators are widely used in cancer
therapy and in x-ray machines for inspecting welds and forgings. Radiation measurement facilities, such
as border inspection portals are often subjected to industrial sources of x rays. Although sources of high-
energy photon radiation are usually well shielded horizontally by thick building walls, they often have
limited shielding provided by a roof and, hence, radiation escaping upwards can scatter in the atmosphere
and contribute to the background radiation at locations far removed from the radiation facility. This source
of background is termed skyshine and requires special techniques to assess its severity [Shultis and Faw 2000].

21.2 Mitigation of the Radiation Background


The design goal for a radiation measurement system is to reduce the background to sufficiently low levels
so that meaningful measurements of a sample can be made and analyzed. For the case of samples with
extremely small activities, the background must be made very low, sometimes to a few counts per day or
per week. Fortunately, most measurement requirements are not as severe. Ideally, the background signals
should be comparable or less than those produced by the sample being analyzed.
In this section the background for gamma-ray and x-ray measurements are primarily considered. To
appreciate the background we all live in, a typical gamma-ray energy spectrum is shown in Fig. 21.7 and the
most often seen contributors to the various full energy peaks seen in such a spectrum are listed in Table 21.6.
The background spectrum of Fig. 21.7 has an overall (sum over all energy channels) of about 35 cps, which
is higher than one might like, but is unavoidable in this measurement laboratory with little protection from
cosmic rays and which also is enclosed by thick concrete walls, floor and ceiling, all containing significant
40
K.
1134 Mitigation of Background Chap. 21

Table 21.6. Full energy gamma-ray peaks observed in a Ge detector


background spectrum. The most intense are indicated by boldface type.

Energy Energy Energy


Origin Origin Origin
(keV) (keV) (keV)

Bi Kα2 74.82 125 Sb 427.9 208 Tl 860.6


Bi Kα1 77.11 228 Ac 463.0 228 Ac 911.2
228 Th 84.40 7 Be 477.5 214 Bi 934.1
Bi Kβ1 87.35 208 Tl 510.7 228 Ac 964.8
Bi Kβ2 89.78 annilation 511.0 228 Ac 969.0
234 Th 92.58 106 Ru 511.8 214 Bi 1120.3
228 Ac 129.1 208 Tl 583.2 214 Bi 1155.2
144 Ce 133.5 214 Bi 609.3 214 Bi 1238.1
228 Ac 153.9 106 Ru 621.8 214 Bi 1281.0
235 U 185.7 137 Cs 661.7 214 Bi 1377.7
226 Ra 186.2 214 Bi 665.4 214 Bi 1401.5
228 Ac 209.3 212 Bi 727.3 214 Bi 1408.0
212 Pb 238.6 228 Ac 755.3 40 K 1460.8
224 Ra 240.9 95 Zr 756.8 228 Ac 1495.9
214 Pb 242.0 95 Nb 765.8 228 Ac 1588.2
228 Ac 270.2 214 Bi 768.4 214 Bi 1729.6
228 Ac 328.0 228 Ac 795.0 214 Bi 1764.5
228 Ac 338.3 214 Bi 806.2 214 Bi 1847.4
214 Pb 351.9 228 Ac 835.7 214 Bi 2204.1
228 Ac 409.5 228 Ac 840.4 208 Tl 2614.5

Source: Gilmore [2008] and Zvara et al. [1994].

Gamma-ray counting facilities can be classified into three broad categories. First ultra-low-level facilities
are characterized by extremely low background count rates, often less than a few counts per day. Such
facilities require heroic effort and expense: detector, electronics, and support material, all constructed from
radiopure materials, are placed deep underground at depths up to 10,000 m (water-equivalent). There are
several tens of these facilities currently in operation most intended to investigate various rare phenomena
such as proton decay, neutrinoless double beta decay, magnetic monopoles, dark matter, neutrino physics,
etc. A few are also used to measure very low levels of radioactivity.
In the second category are very low-level facilities, which use, in addition to passive lead and copper
shielding around the spectrometer, electronic coincidence shielding to suppress the Compton plateau and
the cosmic ray background. Many are placed several hundred to a few thousand meters (water-equivalent)
underground. Background count rates in such facilities can thus be reduced to a few cps. The third
category of counting facilities are at or near ground level and simply rely on passive shielding around the
spectrometer and isolation from man-made radiation sources. These relatively inexpensive facilities typically
have background count rates of several tens of counts per second.
Almost all the peaks seen in Fig. 21.7 are attributable to 40 K and members of the 238 U and 232 Th decay
chains.5 Although not seen in Fig. 21.7, the radionuclide 9 Be (T1/2 = 53.3 d), produced by cosmic rays,
can also sometimes be seen. The fission product 137 Cs, produced by atomic bomb tests, can be seen. Other
background spectra sometimes also show the fission products 95 Zr, 95 Nb, 106 Ru and 144 Ce.

5 These radionuclides are sometimes referred to simply as the KUT nuclides.


Sec. 21.2. Mitigation of the Radiation Background 1135

Figure 21.7. Background energy spectrum obtained over 162.5 h with a 180-cm3 HPGe detector
in the Radiation Detection Instructional Laboratory of Kansas State University. Courtesy of
Nathaniel Edwards, KSU.
1136 Mitigation of Background Chap. 21

Before discussing ways to minimize the effect of background on the analysis of a sample, it must be
recognized that the choice of detector type depends on the specific application. If radionuclide identification
is the purpose, then a high-resolution spectrometer should be selected. However, if detection of contamination
is of interest, then a high-efficiency detector, generally with poorer resolution, should be chosen. In either
case, the larger the active volume the better the statistics for a given count time. Nevertheless, while
increasing the detector size increases the measured foreground counts, it also proportionally increases the
number of background counts. Thus, increasing a detector’s size does little to improve the foreground-to-
background ratio, although it is usually easier to separate the background from a foreground spectrum with
a high-resolution detector such as HPGe compared to a NaI:Tl spectrometer.
There are several ways to improve the foreground-to-background ratio so that the background-corrected
spectrum depends less on the background spectrum. These methods are discussed below.

21.2.1 Sample Placement


To increase the foreground count rate from a sample, the sample should be placed as close to the source
as possible. Unless the sample activity is weak, source placement too close to the source may increase the
deadtime of the detection system beyond acceptable limits. Also the position of a sample with respect to
the detector is further limited if activities of the radionuclides in the sample are sought (as distinct from
just the identification of the radionuclides through the energies of their gamma rays). For absolute counting
it is important that the efficiency of the spectrometer as a function of gamma-ray energy is known. This
energy-dependent efficiency is determined by “point” calibration sources placed at well-defined positions,
typically tens of centermeters on the axis from the detector. Thus samples must be made physically small
and placed at a calibration position to appear as a point source. Sometimes the distance between source
and detector may be very difficult or impossible to change, such as measurement systems designed to study
solar neutrinos and cosmic rays.
If background radiation is weak compared to the sample activity, the source (and detector) should also
be placed as far as possible from walls and other objects from which gamma rays emitted by the source could
be reflected into the detector. The minimization of this reflection contribution when the detector must be
shielded from background radiation is considered in more detail later. Also if a sample is physically large
compared to the detector volume, then corrections must be made to account for photon absorption by the
sample itself, thereby preventing sample radiation from reaching the detector.

21.2.2 Minimize Radioactivity in the Detector System


Because all materials contain radionuclides to a lesser or greater degree, it is important in the construction
of a low-level detection system to use materials with very low radionuclide (RN) concentrations for both the
material that detects the energy of the incident radiation as well as the detector assembly itself.
In Table 21.7 are listed representative specific radionuclide activities in materials commonly used in many
spectrometer systems. Most of the KUT radioisotopes appear as impurities and their concentrations often
vary by factors of ten or more depending on how the materials were prepared. Materials with low levels
of radionuclide contaminants are essential to reduce the background in a spectrometer. This is particularly
true for components that are very close to the detector and include the detector material itself, the casing
of the detector, radiation shields near the detector, the air surrounding the detector, and various system
components such as preamplifiers, photomultipliers, and cryostat endcaps. Selection of materials for low-level
spectrometer systems is a lengthy but vital aspect of the design of a spectrometer system with an inherent
low background. Guidance can be found from published accounts of the construction of systems in existing
facilities such those described by Brodzinski et al. [1985] and Leonard et al. [2008] who also provide specific
radionuclide activities in over 200 materials considered for the EXO-200 facility.
Sec. 21.2. Mitigation of the Radiation Background 1137

Table 21.7. Typical naturally occurring radionuclide concentrations in various


materials used in detector systems.
Average specific activity (Bq kg−1 )
Material
40 K 238 U or 214 Bi 232 Th or 208 Tl

aluminum < 0.4–15 0.07 0.7


< 0.07–35† 0.1–4‡
aluminum (6061 Harshaw) < 0.83 0.7 7.0
aluminum (1100 Harshaw) < 1.0 < 0.28 4.0
aluminum (1100 ALCOA) < 1.8 < 1.8 1.3
aluminum (3003 Harshaw) 9.3 < 0.43 1.7
apiezon grease 5 8 8
berylium 15 120† < 0.2‡
cement, Portland 75 22 4
copper 0.2 0.06 0.04
copper, sheet < 1.7 < 0.013–0.05† < 0.005‡
copper (101) < 0.008 < 0.0008† < 0.0005‡
cooper(OFHC) 0.2 0.015–0.17† < 0.005†
epoxy < 20–120 14–900† 0.8–70†
flint glass 0.1 0.03 0.03
germanium 0.2 0.02 0.02
glass, flint 0.1 0.03 0.03
glass, pyrex 8 0.6 0.8
glass, quartz 35 0.35–17† 0.01–1‡
iron 0.1 0.01 0.01
indium < 0.35 0.05† 0.02‡
lead < 0.02 < 0.0007† < 0.0003‡
magnesium rod 1.7 < 0.67 1.0
MgO 0.4 0.3 0.2
molecular sieve 18–150 6–50 8–75
neoprene 6 < 0.2 < 0.14
plastic tubing < 15 < 0.07† < 0.07‡
polyvinyl resin 3 2 2
printed circuit board 70 70† 35‡
rubber, sponge < 7–35 1.3–200† 1–35‡
silica, fused < 20 < 0.2† < 0.35‡
silicone, foam < 35 1† 0.35‡
sodium iodide < 0.5 < 0.07† < 0.05‡
solder < 0.15 < 0.015† < 0.005‡
steel, stainless < 3.5 < 0.1† < 0.035‡
steel, stainless (304) < 0.33 < 0.12 < 0.10
steel, stainless (304-L) 1.7 < 0.083 < 0.083
steel, pre-WWII < 0.15 < 0.015† < 0.01‡
teflon < 0.35 < 0.002–0.1† < 0.005‡
titanium 0.02 0.06 0.004
† 214 Bi ‡ 208 Tl.

Sources: Zvara et al. [1994], Brodzinski et al. [1985] and Camp et al. [1974].

In gas-filled detectors, the working gas may contain 222 Rn and 220 Rn and their daughters. This con-
tribution to the background can be reduced by purifying the gas or by just letting the gas age for several
half-lives of 222 Rn (T1/2 = 3.38 d). The material of inorganic detectors such as NaI:Tl and CsI:Tl contribute
to the background mainly through 40 K and to a lesser extent through U and Th impurities, although with
modern manufacturing methods these contributors to the background have been largely eliminated. Ger-
1138 Mitigation of Background Chap. 21

manium detectors require a very high degree or purity to produce crystals suitable for radiation spectral
measurements and so background from RN impurities is quite small. Nevertheless, manufacturers of ultra-
low-level spectrometers can, for an additional cost, provide Ge detectors with extremely low concentrations
of impurities. Typically such highly pure crystals have an inherent activity about ten times lower than that
of conventional ones [Zvara et al. 1994].
Bismuth germanate (BGO) crystals can have an appreciable background from the impurity 207 Bi (T1/2 =
38 y), which is thought to be produced by cosmic ray protons in (p,n) reactions with 206 Pb in the same
ore from which the Bi was extracted. BGO produced from lead-free ores does not have this background
component. Some of the newer inorganic scintillators that are presently attractive are compounds containing
lanthanum or lutetium (see Sec. 13.2). However, these elements contain naturally occurring radioisotopes
and, thus, have an inherent built-in background gamma-ray source. To eliminate these radionuclides would
require isotopic separation, an expensive process not routinely available. Consequently, these scintillators
are not well suited for low-level spectrometric applications.
Certain materials such as pyrex glass have KUT radionuclides as normal constituents and, thus, can
be a significant background source. Most materials contain these radioisotopes as impurities and so they
can be reduced by various purification processes. Electrolytic copper and magnesium generally have low
levels of radioactivity and are good choices for the construction of low-background counters. Stainless steel
also generally has low-background activity. However, aluminum, which is widely used structurally for many
experimental systems because of its reasonable cost and ease of cutting and machining, can have relatively
high levels of radioactivity from uranium and/or radium contaminants. Brass also generally has low specific
radioactivities (if its lead content is low). Indeed, one facility replaced stainless steel screws with brass ones
to reduce ever so slightly the background [Brodzinski et al. 1985]. Electric solder and circuit boards often
have high levels of radioactive impurities and, thus, electrical components in a spectrometer system must be
evaluated as a source of background radiation.
Scintillation spectrometers rely on photomultiplier tubes (PMTs), but the glass enclosures of these tubes
and the tube base or socket are often a significant source of radiation background. Manufacturers of PMTs
offer, at a higher price, versions that have significantly smaller radioactive content. Likewise, tube bases
are also available that have much less activity that normal sockets. Detector housings are usually made of
aluminum, magnesium or beryllium for scintillator materials and of stainless steel for gas tube detectors.
These housing materials must be chosen to have the lowest radioactivity possible. Germanium detectors
must be cooled cryogenically for proper operation, and so another possible source of background is the
radioactivity contained in the endcap of the cryostat which is usually positioned adjacent to the Ge crystal.
Material for such endcaps must contain very low levels of radioactivity.
Although not widely used in the construction of radiation spectrometers, materials such as plastics and
carbon fibers, which do not derive from ores, contain extremely low levels of radioactivity. Almost all
radioactivity in these materials comes from the cosmogenic radionuclides of 3 H and 14 C, which emit only
beta particles and, thus, do not contribute to the background in a gamma-ray spectrometer (save through
low-energy bremsstrahlung). Indeed, sample holders and calibration source encapsulations are usually made
from plastic to avoid the introduction of background gamma rays.

21.2.3 Passive Shielding of Radiation Spectrometers


To reduce the background response inherent in any radiation measurement, it is routine to use some sort of
radiation shield to minimize the amount of background radiation that reaches a detector. Shields are usually
composed physically of matter, although shields of a non-corporeal nature could be used. In fact one of
the most important shields for us on earth are magnetic fields produced by the sun and earth that deflect
charged cosmic radiation from our detectors on the earth’s surface. In principle, one could use strong electro
magnetic fields around a detector to shield the detector from incident charged particles.
Sec. 21.2. Mitigation of the Radiation Background 1139

Another extreme shield is to use the earth itself as a shield by moving the detector deep underground in
old mine shafts, for example, to prevent almost all cosmic rays from reaching the detector. This is done in
large research facilities that seek to study neutrinos or seek the half-life for proton decay. Such experiments
have extremely weak foreground signals (some as low as counts per week or even months) and even the
smallest background would swamp the foreground response.
However, for most radiation measurement situations, far less heroic shielding effort is needed to ob-
tain statistically useful results. In the next two sections the use of common shielding materials and their
arrangement to reduce background is discussed.

21.2.4 Shielding Against Gamma Rays


To reduce the background in a gamma-ray spectrometer, passive methods employing photon shields are
almost always used. Because photons are exponentially attenuated as they pass through a shield, unlike
charged particles which have a finite range, no photon shield can stop all photons from reaching the spec-
trometer. However, proper shield design can be quite effective in reducing the spectrometer background.
Lead
Because of its large interaction coefficient (macroscopic cross section) for gamma and x rays, lead (> 99.9%
pure) is routinely used as a shielding material against these radiations. However, lead is a poor construction
material and is not suited for high temperature applications (melting point 327.4◦ C). To increase its strength,
lead is often alloyed with antimony. Lead shields are relatively easy to fabricate because lead may be cast,
extruded, rolled, machined and welded. Casting requires special care because lead increases in mass density
from the liquid at 10.678 g cm−3 to the solid at 11.34 g cm−3 [Kirshenbaum et al. 1961], leading to a volume
decrease of 5.83% upon solidification. Also, the fumes from lead are toxic and safety precautions should be
exercised. Lead is resistant to chemical corrosion, but it is a relatively expensive material (currently about
$2.30 per kg).
Lead often is cast into rectangular bricks (typically, 2× 4× 6 inches) which are then used to create simple
gamma-ray shields by stacking the bricks. Streaming through the cracks between bricks can be minimized
by staggering the brick layout or shaping the bricks so there are no straight line streaming paths through the
shield. Alternatively, lead may be cast into cylindrical annuli to produce 2π shielding without corners. When
casting lead, care must be taken to avoid voids in the cast. Sometimes lead shot is used to fill containers to
produce a lead shield with slightly lower density than solid lead, but with more flexibility in the shape of the
shield. Epoxies and plastic putty-like compounds containing high concentrations of lead are commercially
available which can be molded and shaped to fill shield gaps or shield penetrations through which radiation
could stream.
Lead and uranium are usually found together in ore and, although the uranium and most of its decay
daughters are easily removed upon smelting and purification, the primordial Pb decay daughters are retained
in the lead. Of these 210 Pb (T1/2 = 22.3 y) is of concern for shielding for ultra-low-level gamma-ray
spectrometers because it emits a 46 keV gamma ray followed by 205 and 304 keV gamma rays from the
decay of its daughter 210 Bi. After several hundred years this component of background radiation from a
lead shield disappears through decay. Lead has been extracted and used by humans for several thousand
years. This ancient lead is ideal for constructing shields with low radioactivities for ultra-low-level counting
spectrometers. Although quite expensive, sources of old lead are still sometimes available. Lead, first
obtained as a byproduct of silver extraction from ore, has been used by humans since about 4000 BC.
Romans used it as liners for aquaducts, baths, and almost all other plumbing applications. Later in history,
the building of medieval churches consumed much lead as roof liners, masonry joints and even as mortar.6
6 One source of old lead used for the Italian Cryogenic Underground Observatory for Rare Events (CUORE) was from a Roman
ship that sank between 80 and 50 BC off the coast of Sardinia. From this shipwreck over 1000 lead ingots, each 33 kg in
1140 Mitigation of Background Chap. 21

Water
Large water-filled tanks offer an inexpensive and flexible way to create gamma-ray shields. On a per unit mass
basis, water is almost as effective in reducing the energy of photons through Compton scattering, as is lead.7
Furthermore, water is far less expensive and can be more easily purified to remove essentially all radioactive
impurities save tritium which is of little concern for gamma-ray spectroscopy. Only the radioactive impurities
in the tank materials are of concern. However, lead has a larger photoelectric cross-section and is a superior
material for absorbing low-energy photons. Thus, rather than using a monolithic shield, a layered approach
can be used with a water shield used to reduce the high-energy background gamma rays followed by a thinner
lead shield near the spectrometer system to absorb the low-energy photons.
To reduce the background, the spectrometer could be lowered into water, thereby creating a much larger
water shield. At depths of about 10 meters, the background for surface terrestrial radionuclides and all cosmic
rays (except for muons) are eliminated. Only the radionuclides dissolved in the water and incorporated in
the spectrometer produce a background. This approach has been taken to an extreme with the IceCube
Neutrino Observatory at the Amundsen-Scott South Pole Station in Antarctica where thousands of sensors
are spread over 1 km3 at depths between 1450 and 2450 meters in the Antarctic ice cap. Here the water, in
the form of ice, serves both as the neutrino detection medium as well as a shield against cosmic rays.

Steel
Steel (or iron) is sometimes used to fabricate gamma-ray shields although thicker iron shields compared to
lead shields are needed to produce the same reduction in transmitted radiation. For example, the tenth
thickness8 for 1-MeV photons in iron is almost 5 cm (compared to 1.2 cm in lead and 14 cm in water). Often
a shield has a steel outer layer followed by a thinner inner lead layer.
Steel generally has low concentrations of radioactive impurities and is often a less expensive alternative
to a large lead shield. As mentioned earlier in this chapter, energetic cosmic ray neutrons can lead to
the buildup of radioactive 54 Mn in iron, so steel produced to provide shielding for low-level spectrometers
should be moved underground as soon after production as possible. Also because post WW II steel contains
fission products from open-air nuclear tests in the 1950s, old pre-WW II steel, typically from old ships, is
often sought. But unless stored properly, cosmic ray neutrons may have contaminated this old steel. Also
steel produced from scrap iron may also contain unacceptable radioactive impurities as a consequence of
radionuclide sources being inadvertently included with the scrap iron.

Tungsten
Tungsten, because of its large Z = 74 number and its high density of 19.3 g cm−3 is an excellent material
for gamma-ray shielding. But pure metal is hard to machine or to cast. To form various shapes of tungsten
components, powder technology is often used to produce a sintered product with almost the same density
as the metal. More frequently, tungsten is alloyed with nickel, iron, and copper to produce a metal with a
density of about 90% of tungsten that is far easier to machine. But because of its cost, machinability, and
toxic properties, tungsten is used in limited quantities and usually only for shields adjacent to a source. Its
use in low-level spectroscopy is to produce collimated photon beams in a small space.

weight, were recovered. Italy’s National Institute of Nuclear Physics financially supported the archaeologists in their recovery
efforts and, in return, received 120 of the most damaged ingots from which a 3-cm-thick low-activity shield was constructed
for the underground Laboratory at Gran Sasso.
7 The mass interaction coefficient μ/ρ for 1-MeV photons is 0.07066 and 0.06803 cm2 g−1 for water and lead, respectively.
8 The tenth thickness is the thickness of a material required to reduce the uncollided radiation to 10% of its incident value, and

is given by
x1/10 = ln 10/μ(E),
where μ is the total interaction coefficient for the material for photons of energy E.
Sec. 21.2. Mitigation of the Radiation Background 1141

Table 21.8. Typical compositions of representative concrete after curing.

Partial density (g/cm3 )

Ordinary Ordinary Magnetitea Barytesb Magnetite Limonite Serpentined


Element
(NBS 03) (NBS 04) and steel and steelc
H 0.020 0.013 0.011 0.012 0.011 0.031 0.035
O 1.139 1.171 1.168 1.043 0.638 0.708 1.126
Si 0.342 0.743 0.091 0.035 0.073 0.067 0.460
Ca 0.582 0.194 0.251 0.168 0.258 0.261 0.150
C 0.118 0.002
Na 0.040 0.009
Mg 0.057 0.006 0.033 0.004 0.017 0.007 0.297
Al 0.085 0.107 0.083 0.014 0.048 0.029 0.042
S 0.007 0.003 0.005 0.361
K 0.004 0.045 0.159 0.004 0.009
Fe 0.026 0.029 1.676 3.512 3.421 0.068
Ti 0.192 0.074
Cr 0.006 0.002
Mn 0.007
V 0.011 0.003 0.004
Ba 1.551
Ni 0.026
P 0.007
Density
(g/cm3 ): 2.41 2.35 3.53 3.35 4.64 4.54 2.1
a Magnetite (FeO·Fe2 O3 ) as aggregate.
b Barytes, a BaSO4 ore, as aggregate.
c Limonite, a hydrated Fe O ore, plus steel punchings, as aggregate.
2 3
d Serpentine (3MgO·2SiO ·2H O) as aggregate; a concrete usable at high temperatures with
2 2
minimal water loss.
Source: From Shultis and Faw [2000].

Concrete
Concrete is the most widely used shielding material for both gamma rays and neutrons because it is relatively
inexpensive and, while still a liquid slurry, can be poured into forms to create shields of all shapes and sizes.
It can also be cast into concrete blocks which can later be stacked to form radiation shields. Concrete is
prepared from a mixture, by weight, of about 13% cement, 7% water (including water in the aggregate), and
80% aggregate. There are many different types of concretes each with distinctive properties as determined
by the choice of aggregate [see Shultis and Faw 2000]. For example, to enhance its photon-attenuation
properties, scrap iron or iron ore may be incorporated into the sand-and-gravel aggregate. Examples of
elemental compositions of concrete frequently encountered in radiation shielding applications are given in
Table 21.8.
However, concrete often has appreciable concentrations of the KUT radionuclides. In any spectrometer
facility with concrete walls, floors, and ceilings, the 1.46-MeV gamma ray from 40 K is almost always observed
in a gamma-ray spectrum. From Table 21.8 it is seen that barytes concrete, which is the most effective
concrete for attenuating gamma rays, has the highest K concentration. To reduce the 40 K presence, special
(and expensive) low potassium sand and gravel can be used. However, as seen in Table 21.7, common cements
also have high 40 K activities. To ameliorate the radionuclide impurities in concrete shields, steel, or lead
liners can be placed on the inner surface of a concrete shield.
1142 Mitigation of Background Chap. 21

Mercury and Molybdenum


Like tungsten, mercury also has low intrinsic radioactivity and, because of its high Z = 80 number and
density ρ = 13.53 g cm−3 , is an excellent material for attenuating gamma rays. However, also like tungsten,
it is relatively expensive and because it is a liquid it must be placed in containers, which may themselves be
another source of gamma rays. Mercury is also toxic and thus requires special care in handling. Nevertheless,
shields made from mercury have been used in ultra-low-level counting facilities.
Molybdenum is another material with good gamma-ray shielding properties (Z = 42 and ρ = 10.2 g
cm−3 ). It generally has low intrinsic radioactivity, but like tungsten and mercury is relatively expensive.

21.2.5 Shielding Against Neutrons


Although most gamma-ray spectrometers are inherently insensitive to neutrons, background neutrons are
still of concern in the design of low-level counting facilities. Neutrons produced by cosmic rays have supra-
MeV energies, and as they slow through scattering interactions they produce inelastic scattered gamma rays.
Further these neutrons are eventually absorbed creating highly excited nuclei which decay by the emission
of energetic capture gamma rays. The capture gamma rays are often very energetic, some with energies of
8 to 10 MeV. Also neutrons, particularly after they have slowed, can interact with elements in the detector
itself to produce radionuclides, such as 24 Na in a NaI:Tl detector whose decay produces gamma rays, or
produce reaction products, such as those in the 6 Li(n,t)4 He reaction in Si(Li) or Ge(Li) detectors. Thus,
one must use neutron shielding outside the gamma-ray shielding to minimize the gamma-ray background in
the spectrometer system.
Because neutrons are absorbed mainly when they have near thermal energies, a neutron shield for fast
neutrons first attempts to slow the neutrons through scattering interactions (or moderate them) and then
absorb them with materials such as cadmium, boron, or lithium, that have large thermal-neutron cross
sections. To moderate neutrons rapidly, materials such as water or polyethylene with a high hydrogen
content are normally used because the lighter the scattering nucleus, the more energy a neutron loses on a
scatter. However, for cosmic ray neutrons with energies above 10 MeV, the cross section for scattering from
hydrogen decreases rapidly and becomes ineffective at slowing the neutrons. Consequently,concrete used
for neutron shielding against fast neutrons usually contains high Z materials, such as iron, which slow fast
neutrons through inelastic scattering (and also produce unwanted inelastic scattering gamma rays). Once
the neutrons are slowed below 1 MeV, hydrogen can then quickly moderate the neutrons towards thermal
energies where they are absorbed by impurities or by materials with large neutron absorption cross section
that are added to the moderating material.
From ease of fabrication, fast neutron shields are usually composed of laminates of iron and high density
polyethylene (HDP). As the neutrons approach thermal energies, 6 Li can be incorporated into the HDP
to absorb the slow neutrons without the emission of any capture gamma rays. Often a high Z layer is
added to the inner surface of the neutron shield to attenuate capture-gamma, inelastically scattered, and
bremsstrahlung photons. For instance, cadmium or boron is widely used to absorb thermal neutrons, but
such absorptions produce gamma rays that must be shielded from the detector.

21.2.6 Minimize Radioactivity in Air around Spectrometer


Gaseous radon and its airborne daughters are always present in the air in any low-level counting facility.
Indeed without adequate ventilation these radionuclides can build up, thereby producing air concentrations
many times those in ambient outside air. This is especially a problem for underground facilities. To avoid
this activity in the air in a spectrometer counting cavity two main approaches have been used. One is to
seal the cavity after the sample has been inserted and then wait several days before counting to allow these
Sec. 21.2. Mitigation of the Radiation Background 1143

Table 21.9. Typical naturally occurring radionuclide concen-


trations in various building and structural materials.
Average specific activity (Bq kg−1 )
Material
40 K 226 Ra 232 Th

asbestos 200 10 15
brick, clay (red) 670 50 50
brick, snad-lime 330 10 10
cement 200 20 15
ceramics 500 30 40
clinker 600 60 70
concrete 400 40 30
concrete, aerated 430 60 40
granite 1000 80 80
gravel 150 10 10
limestone 60 10 5
marble 150 10 5
natural gypsum 80 10 10
pearlite 1200 50 80
plaster 250 15 45
phosphogypsum 60 390 20
sand 200 10 10
Source: Eisenbud [1987], UN [1977], and Zvara et al. [1994].

airborne radionuclides to decay. However, this approach severely limits the rate at which samples can be
analyzed because the insertion of a new sample requires a multiday wait before analysis.
The usual approach to minimize airborne radioactivity is to purge the counting cavity with purified gas,
such as argon, which has little inherent radioactivity. Some facilities whose spectrometer requires cryogenic
cooling with liquid nitrogen use the boil-off nitrogen as a purge gas.
Radionuclides from the soil or radon decay can also be attached to dust particles, which also contribute
to the air activity. Thus, it is important to effectively filter the ventilation air to the counting room.

21.2.7 Use Construction materials with Low Radioactivity


Typical concentrations of 40 K, 226 Ra, and 232 Th in common building materials are given in Table 21.9.
However, these activity concentrations can vary by several hundred percent depending on the source of the
material. Typical radionuclide activities in materials used in construction of radiation detection systems are
listed in Table 21.7. Again these activities can vary substantially depending on the manufacturer, but to
minimize the effect of background on radiation spectrometers, it is imperative that close attention be given
to the choice of materials used.

21.2.8 Counting Enclosures


Almost all low-level counting spectrometers and the radioactive sample to be analyzed are placed in some
small enclosure or cavity whose walls act as the primary passive shields against background radiation in the
laboratory walls and air. These cavities typically have a rectangular parallelepiped shape because the walls
are most conveniently constructed from shielding bricks or plates of various materials. Some cavities are
cylindrical in shape with walls made from lead and other materials cast into cylindrical annuli shapes, but
these are more expensive and difficult to fabricate than parallelepipeds. The shield material used for these
cavities should, of course, contain as little radioactivity as possible. The size of the counting cavity is usually
quite small so as to minimize the amount of shielding required.
1144 Mitigation of Background Chap. 21

As background radiation incident on the walls of the counting cavity is attenuated, it also creates a
buildup of secondary radiation in the form of Compton scattered photons, bremsstrahlung, and x rays. Even
if the shield material is radiopure, low-energy photons produced in the shield walls can still enter the counting
cavity. Although lead is a excellent shield material, photoelectric interactions in it from background photons
produce significant low-energy x rays (Kα = 75 keV, Kβ = 84.9 keV, and Lα = 10.5 keV). To absorb these
x rays, lower Z materials, such as copper and aluminum, are often used as inner shields. One example of
a passive shield described by Zvara et al. [1994] is that at the Comenius University in Czechoslovakia has
a mass of 18,000 kg with outer dimensions of 80 × 90 × 172 cm. It is composed, starting from the outside,
with 1 cm of Fe, 10 cm of Pb, 5 cm of Cu, 8 cm of polyethylene with boric acid, 1 mm Cu, and 1 cm of
Plexiglas. To stop the low-energy, non-muonic cosmic rays, the top of the enclosure has a 12-cm Fe slab
shield. Modern materials with no special selection were used.
As an illustration of the use of a Cu inner liner to reduce Pb x rays, the energy dependent flux of 60 Co
photons leaving a 10-cm bare and 0.5-cm Cu clad lead shield is shown in Fig. 21.8. The flux shown is that
entering a NaI:Tl crystal on the cold side of the shield. No Gaussian smearing of the spectrum is used to
account for the actual resolution of the detector. Notice the Cu liner totally eliminates all the Pb x rays as
well and also suppresses some of the transmitted Compton lead scattered photons, except near the Pb x ray
region where the Cu slightly enhances the photon flux. With modern radiation transport codes, calculations
such as those in Fig. 21.8 can be used to design shields for counting cavities and can eliminate much of
the trial and error and intuition used a few decades ago to design passive shielding for low-level counting
facilities.
In measuring the spectrum emitted by a sample with small amounts of radioactivity, radiation from the
sample that reflects from the inside of the passive shielding is usually not of too much concern. However,
such radiation incident on the inner portions of a lead shield will produce x rays that will be seen by the
spectrometer. Again, lining the inner cavity with lower Z materials can ameliorate this effect. An example
of the reflected photon flux from 137 Cs gamma rays emitted by a sample is shown in Fig. 21.9. Here it is
seen that a 0.5-cm-thick Cu liner almost totally eliminates the lead x rays but at the price of significantly
enhancing the low-energy part of the reflected spectrum. Such calculations with modern radiation transport
codes should be used to customize the inner cavity shielding for a particular type of radiation source that is
to be analyzed.

21.2.9 Laboratory Location


Terrestrial and cosmic ray background are greatest at the earth’s surface. Consequently, construction of a
low-level spectrometer facility at ground level is seldom done. Even a few tens of meters below the surface,
the background radiation is greatly reduced, although the cosmic-ray muonic component is affected little.
Thus, in a multistoried building, the low-level spectrometer system should be built in the lowest basement
room possible.
Cosmic ray background can be almost completely eliminated by building the counting system deep
underground or underwater. To this end, there are several tens of low-level counting systems around the
world that have been built in abandoned mines, some of which are close to 10,000 m (water equivalent) deep.
At such depths all the muons are stopped, leaving only neutrinos, which are the particles being studied
in many of these facilities. Of course, the walls of underground caverns or rooms still contain primordial
radionuclides so that spectrometer shielding is still required. Ideally, surrounding wall material should have
as small as possible radionuclide content. For this reason, abandoned salt mines are very attractive locations.
Shown in Fig. 21.10 are the background spectra for four different low-level facilities, two at ground level and
two deep underground away from cosmic ray muons. The superiority of an underground location is obvious.
Sec. 21.2. Mitigation of the Radiation Background 1145

Figure 21.8. 60 Co gamma rays transmitted through 10 cm of lead and from


the same amount of lead plus 0.5 cm of copper on the exit surface as calculated
by MCNP6. Gamma rays are normally incident on the outer surface.

Figure 21.9. 137 Cs 0.6617-MeV gamma rays reflected from 10 cm of lead and
from the same amount of lead plus 0.5 cm of copper on the reflecting surface
as calculated by MCNP6. The gamma rays are normally incident on the inner
shield surface.

21.2.10 Other Considerations


The measurement of background spectra from low-activity sources almost always requires long count times,
sometimes of multiday or, in extreme cases, multimonth duration. For such long count times, there are a
1146 Mitigation of Background Chap. 21

Figure 21.10. Comparison of Ge:Li background spectra in above


ground (Milano and Kiev) and underground (Mont Blanc and
Solotwino) laboratories. Data are from [Zvara et al. 1994].

myriad of small factors that can affect the spectrometer system and confound the subsequent analysis of
the measured spectra. It is essential that stability of the system be maintained during long data collection
times. It is always a good practice to interrupt a long accumulation time of a spectrum and perform periodic
calibration verifications and recalibrations if necessary.
The response of the electronics is often susceptible to small changes in the ambient temperature. For
example, Rizzacacca [1986] reports that a temperature change of 2◦ C over a 24-hour period can shift the
spectrum from a Ge:Li detector by about one FWHM (2 keV at 1.33 MeV). Today the use of electronic
spectrum stabilizers reduces such shifts substantially. Also underground facilities are less susceptible to
temperature changes because the huge thermal inertia of the surrounding rock and soil minimizes any
temperature fluctuations.
Also during long count times, the background radiation field can fluctuate. This is of particular concern
for the airborne radionuclides of radon and its daughters. Following rain storms or thawing cycles, the
emission of radon from soil and rocks may increase substantially and, depending on how readily airborne
contaminants can reach the gas surrounding the spectrometer detector, the count rate can be affected.
Likewise, activity such as housekeeping activities can alter the concentration of radionuclides in the air.
It stands to reason that any low-level counting facility be located as far as possible from known sources
of radiation such as industrial x-ray sources or other sources used for industrial or research purposes. It is
not a good idea to store even weak radioactive “check” sources or radioactive samples near the spectrometer.
The authors are amazed at how often they have found radiation sources in desk drawers or on shelves in or
near a room used for spectroscopic measurements. It should also be remembered that people are radiation
Sec. 21.3. Self-Absorption of Photons 1147

sources (notably from 40 K) and they also act as radiation reflectors and shields. Thus, their presence in and
around a spectrometer as it collects data alters the background. Such human activity near a spectrometer
can perturb the measured spectrum depending on the effectiveness of the passive shielding surrounding the
spectrometer.
Finally, it should be mentioned that contamination of surfaces near and on the spectrometer can occur
over time, especially if many unsealed calibration sources and/or samples have been processed. Periodic
wipes and checks for such contamination should be made and appropriate remediation taken if such contam-
ination is found. Sometimes sensitive detector windows are protected by plastic film that can be replaced if
contamination occurs.

21.3 Self-Absorption of Photons


So far in the discussion about reducing the background in photon spectrometers, the emphasis has been on
reducing the radiation reaching the spectrometer detector and radioactive content of various components
of the low-level counting facility. However, a radioactive impurity in some facility component does not
necessarily lead to a background count. The radiations from a radioactive decay in some material may be
absorbed in the material before they can escape and deposit their energy elsewhere. This self-absorption
effect can be important in assessing the effectiveness of thick shields and walls of the spectrometer facility.

21.3.1 Infinite Slab


Consider a homogeneous slab shield of thickness T which contains a uniform volumetric source of a radionu-
clide which emits a gamma ray of energy Eo per decay. The number of photons escaping the slab without
interaction is, by symmetry, the same for either surface. The probability the gamma ray escapes through
one surface is [Case et al. 1953]
1 1
P1o (T ) = − E3 (μT ) , (21.3)
2μT 2
where μ is the total interaction coefficient for photons of energy Eo and E3 (x) is the exponential integral
function of order three.9
The one-sided escape probability of Eq. (21.3) can be approximated to within 1% by
$
1 2.077 + 2.951μT + 0.1348(μT )2, 0.003 < μT < 3.5
= . (21.4)
P1o (T ) 4μT, μT ≥ 3.5

The uncollided escape probability for the slab, i.e., through either face is P0 = 2P1o . The uncollided escape
probability is independent of the slab material and depends only on the thickness of the slab in units of
mean free path lengths μ(Eo )T .
Also leaving a slab surface are secondary photons produced by the decay gamma ray interacting in the
slab to produce fluorescence, bremsstrahlung, Compton scattered photons, and annihilation photons. These
photons have a distribution of energies. The total number of secondary photons escaping through one surface,
per source gamma ray, is denoted by P1s . No analytic expression is known for the energy distribution or total
number of these secondary photons. However, with modern transport codes, it is a fairly simple matter to

9 The exponential integral function of order n is defined as


 ∞
En (a) = x−n e−ax dx, n = 0, 1, 2, . . . .
1
1148 Mitigation of Background Chap. 21

make such calculations. In Fig. 21.11 results for a concrete slab are shown. Of particular note is the relative
insensitivity of P1s to the energy of source gamma rays. Unlike P1o , P1s depends not only on the mean free
path thickness of the slab, but it also depends on the slab material because the interaction coefficients for
the various reactions that produce secondary photons vary with the material.

Figure 21.11. One-sided escape probabilities from


a concrete slab for a monoenergetic, isotropic, uni- Figure 21.12. The current or flow rate of photons
formly distributed, gamma-ray source. Concrete is through a unit area of the surface of a concrete shield
ANSI/ANS-6.6.3 standard concrete with a density containing a unit strength volumetric source (Sv = 1
of 2.3 g cm−3 . The solid line is calculated from cm−3 s−1 ) of monoenergetic photons of energy Eo .
Eq. (21.3) and the data points for secondary photons The solid lines for Jno are from Eq. (21.5) and the
were calculated by MCNP6. data points are values obtained with MCNP6.

For a radioactive contaminant that emits gamma rays of energy Eo and that is uniformly distributed
in the slab, the volumetric gamma-ray source strength is Sv = Af cm−3 s−1 , where A is the activity
concentration Bq cm−3 and f is the gamma-ray frequency, i.e., the probability a gamma ray of energy Eo
is emitted per decay. Then the total flow of uncollided photons crossing a unit area on the surface of the
slab is the photon current leaving the slab and is given by Jno = Sv T P1o(T ), where Sv T is the total number
of gamma rays of energy Eo emitted per unit time in a 1 cm2 prism of length T . If gamma rays leave this
prism while migrating in the slab they are compensated, by symmetry, by gamma rays that enter the prism.
Thus, the uncollided current leaving the slab is from Eq. (21.3)

Sv 1
Jn ≡
o
n•Ωφ(Eo , Ω) dΩ = − E3 (μT ) , (21.5)
n•Ω>0 2μ 2

where n is the outward normal to the slab surface. Likewise the flow through a unit area on the slab’s surface
is Jns = Sv T P1s . In Fig. 21.12 these surface flows of escaping photons for a unit strength source strength, i.e.,
Sv = 1. Notice for shields greater than a few mean free paths thick, these surface flow rates become almost
independent of the shield thickness.
The uncollided flux at a point exterior to the slab is [Shultis and Faw 2000]

Sv
φo = [1 − E2 (μT )] . (21.6)

Sec. 21.3. Self-Absorption of Photons 1149

This result assumes that the photons, once outside the slab, no longer interact. Notice the uncollided flux
is not dependent of the distance to the slab surface.
The above analysis is for an infinite slab. However, all slab shields are finite in all dimensions. But if
the point of interest on the surface of the slab is a few mean free paths away from the slab edges, the above
results serve as a good (conservative) approximation.

Example 21.1: A concrete wall 30-cm-thick contains 40 K with a specific activity of 250 Bq kg−3 . The
total interaction coefficient for the 1.46-MeV gamma ray emitted by 40 K is 0.1212 cm−1 and the concrete
has a mass density of 2.3 g cm−3 . Estimate the number of uncollided and secondary photons that escape
per unit time through a unit area on the concrete wall.

Solution:
The radionuclide 40 K emits a 1.46-MeV gamma ray with a frequency of 0.107 per decay. Thus, the
volumetric source strength is
Sv = 250 Bq/kg × 0.001 kg/g × 2.3 g/cm3 × 0.107 = 0.0615 cm−3 s−1 .
The wall thickness in mean free path lengths is μT =(0.1212 cm−1 )(30 cm) = 3.636. The one-sided escape
probability from a concrete slab is, from Fig. 21.11, about P1o = 0.06 or from Eq. (21.3) is found to be
P1o = 0.068176. The approximation of Eq. (21.4) gives P1o = 0.06855. Thus, the number of uncollided
photons escaping is
Jno = T Sv P1o = (30 cm)(0.0615 cm−3 s−1 )(0.068176) = 0.126 cm−2 s−1 .
Alternatively, from Fig. 21.12 Jno for Sv =1 is about 2.0. Multiplication by Sv = 0.0615 gives Jno = 0.123
cm−2 s−1 .
The flow of secondary photons for Sv = 1 is found from Fig. 21.12 to be about 4.1 cm−2 s−1 . Multipli-
cation by Sv = 0.0615 gives Jns = 0.252 cm−2 s−1 .

21.3.2 Infinite Cylinder


Analytic expressions are known for the uncollided escape probability for other simple geometric shapes such
as spheres, hemispheres, oblate spheroids, and cylinders [Case et al. 1953]. Of interest here are impurity
radionuclides in a cylindrical crystal. For a infinite cylinder of radius R, the uncollided escape probability is
"
2μR
P0 (R) = 2 [μaK1 (μR)I1 (μR) + K0 (μR)I0 (μR) − 1]
3
#
K1 (μR)I1 (μR)
+ − K0 (μR)I1 (μR) + K1 (μR)I0 (μR) , (21.7)
μR
where In and Kn are the modified Bessel functions of the first and second kind and of order n. For radii
small compared to a mean free path length 1/μ, Eq. (21.7) may be approximated by
"    #
4μR 1 2 5
P0 (a)  1 − 2
+ (μR) ln + −γ , (21.8)
3 2 μR 4
where γ = Euler’s constant = 0.577216 . . .. For a much larger than one mean free path length
1 3
P0 (a)  − . (21.9)
2(μa) 32(μa)3
1150 Mitigation of Background Chap. 21

For a cylindrical crystal of height 2H and radius R that is uniformly contaminated by a radionuclide
emitting photons of energy Eo , the uncollided flux on the axis at the center of the crystal is given by [Shultis
and Faw 2000]
Sv
φo = G2 (μH, μR), (21.10)
μ
where the function G2 is defined as
 a 
1
G2 (a, b) ≡ [E1 (x) − E1 ( x2 + b2 )] dx, (21.11)
π 0

and which must be evaluated numerically. This function is shown in Fig. 21.13.

Figure 21.13. The function G2 (a, b) used for the calculation


of the uncollided flux at the center of a cylinder of radius
b = μR and height a = 2μH in mean free pathlengths.

21.4 Electronic Methods for Background Reduction


To substantially reduce cosmic ray background generally requires massive amounts of “passive” shielding
with radiopure materials and/or the placement of the spectrometer deep underground where the overlying
earth provides the needed massive passive shield. An alternative is to use “active” shielding techniques in
which multiple detectors and associated electronics are used to reduce the recorded background. Coincidence
and anti-coincidence methods were introduced in Section 20.7.3, with examples of the effectiveness of the
technique (see Figs. 20.27 and 20.28).
Sec. 21.4. Electronic Methods for Background Reduction 1151

21.4.1 Anti-coincident Background Reduction


Active (anti-coincidence) shielding is a powerful method for reducing the detector background. This method
uses several detectors placed near the spectrometer detector to reject a spectrometer detector pulse that
coincides within a microsecond or so of a pulse originating in one or more of the surrounding detectors. Such
coincident pulses arise from Compton scattered gamma rays from the passive shield or spectrometer detector.
Likewise cosmic rays may produce nearly simultaneous pulses in both the spectrometer and a surrounding
detector. Thus, not only is the background reduced, but the Compton continuum in the spectrometer is also
reduced.
An active anti-coincidence shield can be devised using GM-tubes, proportional counters, plastic or liquid
scintillators, NaI:Tl or BGO crystals. If the anti-coincident system is placed inside a passive shield enclosure,
then NaI:Tl detector(s) are attractive because they generally have smaller space requirements and have a
high detection efficiency. The random direction of gamma rays from the environment calls for a uniform
anti-coincidence shield around the spectrometer detector. Cosmic ray muons are quite anisotropic, but do
not significantly affect the required shape of the active shield. This outcome is mainly due to the fact that
a muon path length of only a fraction of a centimeter, is generally sufficient to produce a usable pulse in the
guard detector(s) for the anti-coincidence circuit to reject a spectrometer event.
The Compton scattering process in the detector produces a continuum spectrum that raises the lower
detection limit for gamma rays within this continuum spectrum. The scattered photons that escape the
spectrometer detector can be detected with a sufficiently large NaI:Tl or BGO crystal surrounding the
detector. NaI:Tl has a better energy resolution than that of BGO, but a lower density. As a result NaI:Tl
is about 2.5 times less efficient than BGO (averaged over several common gamma-ray energies) at detecting
the Compton scattered photon. Because BGO has only about 10–20% the light output of NaI:Tl, it has a
higher threshold that consequently causes a lower Compton suppression factor at low gamma-ray energies.
If an HPGe spectral detector is placed above the center of a large anti-coincidence NaI:Tl crystal (30×30
cm), a Compton suppression factor of about 10–12 can be achieved for gamma-ray energies below 1.5 MeV
[Zvara et al. 1994].

21.4.2 Coincident Counting


Many radionuclides emit two or more radiation quanta upon decay. With the use of coincidence counting
techniques using multiple detectors, the background count rate in the spectrometer detector can be sharply
reduced. Only if the spectrometer and another detector both detect an event at the same time is the event
recorded. Although background events are thus most rejected, some events which should be recorded are
rejected because only the spectrometer detector experienced the event. Thus, the efficiency of coincident
counting usually reduces the efficiency of the spectrometer for the radiation of interest while at the same time
much of the background is eliminated. There are several types of coincidence schemes as briefly mentioned
below.
Double Coincidence Spectrometer
This type of spectrometer is used to measure the activity of a radionuclide that emits two or more nearly
simultaneous gamma rays. 60 C for example is one such radionuclide which upon beta decay to 60 Ni, 99+% of
the time emit both a 1.173-MeV and 1.333-MeV gamma ray within 0.7 ps of each other. Usually two NaI:Tl
crystals, a NaI:Tl and HPGe detector or two HPGe detectors, are used. The HPGe-NaI:Tl spectrometer,
which combines the good energy resolution of the HPGe crystal with the high efficiency of the NaI:Tl
detector, is preferred for low-level gamma-ray activity.
Triple Coincidence Spectrometer
This type of spectrometer is used as a pair spectrometer for the simultaneous measurement of the annihila-
tion and gamma photons of radionuclides that decay by positron emission. Three NaI:Tl detectors or two
1152 Mitigation of Background Chap. 21

NaI:Tl detectors with one HPGe detector are combined for this type of spectrometer. Sometimes a large
NaI:Tl crystal split into two optically isolated regions is used, which can also be used as an anti-Compton
spectrometer. A triple coincidence scintillation spectrometer with active and passive shields has been used
for the measurement of 22 Na, 26 Al, and 60 Co activities in meteorite samples [Vartanov and Samojlov 1975].
With this spectrometer, the sensitivity for 22 Na was greatly increased in the presence of higher 26 Al and
60
Co activities.
Beta-Gamma Coincidence Spectrometer
If a sample has a radioisotope that emits two different types of radiation that can be measured simultaneously,
then coincident techniques between the detectors for each type of radiation can be used to substantially
reduce the background signal. For example, many radionuclides decay by beta particle emission whose
excited daughter nucleus decays almost immediately by emitting one or more prompt gamma rays that
are unique to the parent [Dewaraja et al. 1994]. The sample is placed adjacent to a beta counter and a
gamma-ray spectrometer detector. By recording only those events which coincidentally produce signals in
each detector, the background is reduced by eliminating events for which only one detector responds.

PROBLEMS
1. The muons μ− and μ+ are produced by cosmic ray interactions in earth’s atmosphere miles above the
surface. These particles are radioactive with a half-life of 1.523 μs and travel at speeds of β = 0.9997c.
Thus half of the muons decay after traveling (1.523 × 10−6s)(3 × 108 m/s)  450 m. How then do muons
reach the earth’s surface and contribute to our background dose?

2. At what speed must a 58-g tennis ball travel to have a kinetic energy equal to that of the most energetic
cosmic rays, protons with energies of about 1020 eV. How high would the tennis ball jump if 1020 eV of
energy were converted into gravitational potential energy?

3. The energy-dependent neutron flux produced by cosmic rays at ground level which has a water fraction
 .1eV
of 25% is shown in the table below. Estimate the total thermal flux φT = 0 φ(E) dE in units of cm2
h−1 .
E φ(E) E φ(E)
MeV cm−2 s−1 MeV−1 MeV cm−2 s−1 MeV−1
1.13E-08 5.22E+04 4.50E-08 5.41E+04
1.42E-08 5.83E+04 5.66E-08 4.30E+04
1.79E-08 6.32E+04 7.13E-08 3.05E+04
2.25E-08 6.61E+04 8.97E-08 1.89E+04
2.84E-08 6.59E+04 1.13E-07 1.00E+04
3 .57E-08 6.19E+04

4. From the data in Fig. 21.1, how many muons per minute with energies between 100 and 1000 MeV enter
a 4×5 inch NaI:Tl detector near the ground at an elevation of 2493 ft?

5. Potassium and sodium are both Group I elements and thus have similar chemical properties. As a
consequence, K is a natural impurity found in NaI:Tl crystals. Estimate the concentration of K in ppm
(by mass) to produce two cps in a NaI:Tl detector.

6. (a) What is the activity from the decay of 238 U in a 1-kg sample of uranium? (b) what is the total
activity in the sample? State any assumptions made.
Problems 1153

7. Consider a two-storied house 20 × 20 m in size with walls 8 m high and a basement 3 m deep. The
basement floor and walls are of concrete 30-cm thick, and the outside walls are brick 1-cm thick. Plaster
1-cm-thick lines along all walls and the ceilings. Estimate the activity in Bq of 40 K, 226 Ra, and 232 Th
in the structural material of the house.

8. You are responsible for determining the activity of material to be used to create a very low-level gamma
spectrometer facility. You have access to both a HPGe spectrometer and a large NaI:Tl spectrometer.
Explain how you would go about determining the specific gamma-ray energies and emission rates and
the radionuclides impurities of the construction and shield materials being delivered to the facility.

9. Show that for very thin slabs (μT → 0), Eq. (21.3) reduces to P1o = 0.5. Explain why this result should
be expected.

10. Plot the probability that a monoenergetic photon produced by a radionuclide uniformly distributed in
an iron slab escapes uncollided through one side of the shield as a function of the photon energy from
0.1 to 10 MeV. Consider iron slabs of thicknesses 0.5, 1 and 2 mfp.

11. Explain in words why most of the variation in Jno and Jns in Fig. 21.12 occurs in the first few mean free
paths of the slab’s thickness.

12. Twenty percent of the 1.46-MeV gamma rays produced by the radioactive decay of 40 K uniformly
distributed in a concrete slab are found to escape uncollided (half from one side and half from the
other). Estimate the thickness of the concrete slab.

13. Uncollided 40 K gamma rays from a thick concrete wall are measured to be 3.2 per second per cm2 of
the wall surface. Estimate the activity concentration in the concrete in units of Bq/kg.
14. The MCNP6 code used to generate data for Fig. 21.11 and Fig. 21.12 is shown below.

Esc. prob. from infin. slab, w/ uniform isotropic src.


c For standard concrete 1 mfp at 0.5 MeV = 4.98833 cm
c *** cell cards ***
1 1 -2.32 10 -20 -99 imp:p=1 $ slab
2 0 -10 -99 imp:p=0 $ left void
3 0 20 -99 imp:p=0 $ right void
50 0 99 imp:p=0 $ graveyard

c *** surface cards ***


10 px 0.0 $slab left face
20 px 4.98833 $slab right face
99 so 100000. $graveyard sphere

c *** block three -- problem definition


NPS 1000000
MODE P
PHYS:P 10.0 0 0
c
c ----- Src uniform 0 to 1 mfp
SDEF X=d1 Y=0 Z=0 ERG=0.500 PAR=2
SI1 0.00001 4.98833
SP1 -21 0
c
c ----- Detectors: F1 current (uncollided and collided)
F1:p 10 20 T
FT1 INC $ separate by no. scat.
1154 Mitigation of Background Chap. 21

FU1 0 10000 T $ 0 scat; <=10000 scat; total


c
c CONCRETE: ANSI/ANS-6.4.3; rho = 2.32 g/cm^3 mass frac.
m1 1001 -.0056 8016 -.4983 11023 -.0171
12000 -.0024 13027 -.0456 14000 -.3158
16000 -.0012 19000 -.0192 20000 -.0826
26000 -.0122

Modify this input deck to calculate the escaping gamma flux of 0.5-MeV photons by using the f2 tally.
Note that you must use an FM card to multiply the tally by slab surface area to obtain flux per unit
volumetric source. Check your results by comparing the uncollided flux to that of Eq. (21.6).

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GILMORE, G.R., Practical Gamma-Ray Spectroscopy, 2nd Ed., Park, IL: Am. Nucl. Soc., 2000.
New York: Wiley, 2008. SHULTIS, J.K. AND R.E. FAW, Fundamentals of Nuclear Science
HAFFNER, J.W., Radiation Shielding in Space, New York: Aca- and Engineering, 3rd Ed., Boca Raton, FL: CRC Press, 2017.
demic Press, 1967.
UN, Report of the United Nations Scientific Committee on the
ICRP, Report of the Task Group on Reference Man, Interna- Effects of Atomic Radiation, New York, 1977.
tional Commission on Radiological Protection, Report 23, Ox-
ford: Pergamon Press, 1975. UN, Report of the United Nations Scientific Committee on the
Effects of Atomic Radiation, New York, 1982.
KIRSHENBAUM, A.D., J.A. CAHILL, AND A.V. GROSSE, “The Den-
sity of Liquid Lead from the Melting,” J. Inorganic & Nucl. UN, Report of the United Nations Scientific Committee on the
Chem., 22, 33–38, (1961). Effects of Atomic Radiation, New York, 1988.
KOCHER D.C., Radioactive Decay Data Tables, Report VARTANOV, N.A. AND P.S. SAMOJLOV, Applied Scintillation
DOE/TIC-11026, Washington, DC: US Dept. of Energy, 1981. Gamma-Spectroscopy, (in Russian), Moscow: Atomizdat, 1975.
LEONARD, D.S. AND 56 COAUTHORS,“Systematic Study of Trace ZVARA, P., P. OVINEC, AND L. YKORA, “Determination of Very
Radioactive Impurities in Candidate Construction Materials for Low Levels of Radioactivity,” Pure & Appl. Chem., 68, No. 12,
EXO-200,” Nucl. Instru. Meth., A591, 490–504, (2008). 2537–2586, (1994).
Chapter 22

Nuclear Electronics

Despite many great achievements in the science of radio and electronics,


what we know today is far less than what we have still to learn.
David Sarnoff

The bulk of this textbook has been dedicated to the description of radiation detectors and their functional
operation. However, it would seem incomplete not to discuss, at least cursorily, some of the common
electronics used to operate these detectors. Because the field of radiation detector electronics is vast, a
complete and thorough examination of the art is simply not possible in this book, and the authors refer
the reader to other respected works on the topic, including Gillespie [1953], Chiang [1969], Kowalski [1970],
Nicholson [1974], and Spieler [2005]. What follow are brief introductory descriptions of the electronics often
used with radiation detectors and how these electronic circuits operate.
In Sec. 2.4 a brief historical review was presented about the reason for and development of modular
units for nuclear radiation detection. From this early attempt at standardizing detector electronics, Nuclear
Instrument Modules (NIM) were developed. These modules are typically inserted into a universal power
supply unit called a Nuclear Instrument Module BIN (or NIM bin). This system has a set of standards,
described in U.S. DOE Report ER/DOE-0457T, which specifies a 10-volt processing limit. Pulses greater
than 10 volts are rejected or “clipped” upon entering any of the NIM units.
The NIM system is not the only electronic system available. Perhaps the second most popular modular
system is Computer Automated Measurement and Control (CAMAC) system. Analogous to the NIM bin,
CAMAC instruments are powered by a CAMAC crate. CAMAC is popular for circumstances requiring
complicated timing and measurement controls, such as with high-energy collider experiments. Moreover,
CAMAC components are not restricted to only complicated radiation measurements but can be used in
other electronic applications. But because of the typically higher cost of CAMAC components compared to
NIM components, they are usually used only when NIM electronics are less effective. Besides the NIM and
CAMAC systems there are stand-alone units, such as those found in survey instruments, which have multiple
integrated electronic components, all combined within a single unit. In NIM and CAMAC systems, these
different components are separate components. Regardless of the system, the basic electronics described in
this chapter are universally applied within the various electronic systems.

22.1 Mathematical Transforms


Before electronic networks and components are discussed, it is first necessary to briefly discuss the traditional
methods used to mathematically analyze a network of passive elements. Consider a circuit with an input
signal fin (t), be it a voltage or current, to which the resulting output fout (t) is sought. Generally the relation
between the input and output is described by a set of time-dependent ordinary differential equations. Rather
than solve these equations explicitly, they are often first transformed by either a Fourier or Laplace integral
transform. Under such a transform or mapping, the system of differential equations is converted to a set of

1155
1156 Nuclear Electronics Chap. 22

coupled linear algebraic equations. In essence a calculus problem is transformed into an algebraic problem,
which is much easier to solve than are the differential equations. Once the transformed output is obtained
by algebraic means, it can then be mapped back to the time domain by an inverse integral transform to give
fout (t). The two most common transforms used to describe linear circuits are the Fourier and the Laplace
transforms.

22.1.1 The Fourier Transform


The Fourier transform is a generalization
∞ of a Fourier series for functions f (t) that have no periodicity. If
f (t) is absolutely integrable, i.e., −∞ |f (t)| dt < ∞ then the Fourier transform F (ω) of f (t) is given by
 ∞
F (ω) ≡ F[f (t)] = e−jωt f (t) dt (22.1)
−∞

and the inverse transform by


 ∞
1
f (t) ≡ F −1 [F (ω)] = ejωt F (ω) dω, (22.2)
2π −∞

where j ≡ −1 and ω is the angular frequency.1 Here F [f (t)] transforms f (t) from the time domain to the
frequency domain and F −1 [F (ω)] transforms F (ω) back from the frequency domain to the time domain.

22.1.2 The Laplace Transform


Often f (t) is not absolutely integrable (e.g., f (t) is any polynomial in t or f (t) is a step function H(t)).
However, the modified function e−σt f (t)H(t), with σ real and positive, may be integrable, i.e.,
 ∞
dt e−σt |f (t)| < ∞.
0

Then instead of taking the Fourier transform of f (t) (which does not exist), we take the Fourier transform
of " −σt
e f (t), if t ≥ 0
g(t) = (22.3)
0, if t < 0
The Fourier transform of this function and its inverse are
 ∞
F [g(t)] ≡ G(ω) = e−jωt e−σt f (t) dt, (22.4)
0

and  ∞
1
F −1 [G(ω)] ≡ g(t) = ejωt G(ω) dω. (22.5)
2π −∞
This pair of transforms can be simplified by introducing a complex variable s = σ + jω. Clearly,
ω = (s − σ)/j and dω = −j ds. Hence for t > 0
 ∞
1
g(t) ≡ f (t)e−σt = ejωt G(ω) dω
2π −∞
 ∞  ∞   ∞
1   −j σ+j∞

= ejωt f (t ) e−σt e−jωt dt dω = ds est e−σt f (t ) e−st dt ds
2π −∞ 0 2π σ−j∞ 0

1 Although

the usual mathematical symbol is i = −1, the √ letter i is also commonly used in electrical engineering calculations
for current. To avoid confusion, it is common to use j for −1 in circuit theory.
Sec. 22.1. Mathematical Transforms 1157
Table 22.1. Some commonly encountered Laplace transforms.

F (s) f (t) F (s) f (t)


1 s−a
H(t) unit step fn eat cos bt
s (s − a)2 + b2
1 tn−1 s2 − a2
( n = 1,2,...) t cos at
sn (n − 1)! (s2 + a2 )2
Γ(k) 1 1
(k > 0) tk−1 (1 − cos at)
sk s(s2 + a2 ) a2
1 1 1
eat (at − sin at)
s−a s2 (s2 + a2 ) a3
1 1 1 1
(eat − ebt ) (sin at − at cos at)
(s − a)(s − b) a−b (s2 + a2 )2 2a3
s 1 s 1
(aeat − bebt ) sin at
(s − a)(s − b) a−b (s2 + a2 )2 2a
1 1 s2 1
sin at (sin at + at cos at)
s2 + a2 a (s2 + a2 )2 2a
s 1 1 a
cos at e t sin bt
s2 + a2 (s − a)2 + b2 )2 b
1 1 s−a
sinh at eat cos bt
s2 − a2 a (s − a)2 + b2 )2
s s 1
cosh at sin at sinh at
s2 − a2 s4 + 4a4 2a2

or  
σ+j∞ ∞
1 
f (t) = e st
f (t ) e−st dt ds. (22.6)
2πj σ−j∞ 0

From this identity, one identifies the transform pair, known as the Laplace Transform,
 σ+j∞
1
f (t) = est F (s) ds ≡ L−1 [F (s)] (22.7)
2πj σ−j∞
 ∞
F (s) = f (t)e−st dt ≡ L[f (t)]. (22.8)
0
∞
Here σ is a sufficiently large and positive constant chosen so that 0 e−σt |f (t)| dt < ∞. The Laplace
transform is particularly useful for functions f (t) that are zero for negative t.
Unlike that for Fourier transforms, the inversion of the Laplace transforms from Eq. (22.7) is not straight-
forward because it involves contour integration in the complex s-plane. An alternative is to prepare a ‘dic-
tionary’ of Laplace transforms of common functions and, when faced with the need to invert a transform,
simply look up in the dictionary the parent function that has the transform of interest. An example of such
a listing is given in Table 22.1. Perhaps the most complete listing of Fourier and Laplace transforms and
their inverses is that of Bateman [1954].

Example 22.1: Find the Fourier and Laplace transforms for the function
"
0, if t < 0
f (t) =
e−at , if t ≥ 0
1158 Nuclear Electronics Chap. 22

Solution:
The Fourier transform is
 ∞
−1 −(α+jω)t ∞ 1
G(ω) = F[f (t)] = e−αt e−jωt dt = e  = .
0 α + jω 0 α + jω
The Laplace transform is
 ∞ 
−1 −(α+s)t ∞ 1
F (s) = L[f (t)] = e−αt e−st dt = e  =
0 α+s 0 α+s
In this case the results are very similar for the Fourier and Laplace transforms. The general naive, and
incorrect, impression may be that jω in the Fourier transform can be switched for s in the Laplace transform,
and vice versa. However, this is actually not always true, and in fact, the Fourier transform is a smaller
subset of the Laplace transform with the term σ = 0.

22.1.3 Properties of the Laplace Transform


The Laplace transform has many useful properties that are used throughout this chapter. These properties
are summarized below. The Fourier transform, likewise, has many similar properties.
Integration:
 t
1 F (s)
L dt f (t ) = L[f (t)] = . (22.9)
0 s s
t
Example: Given f (t) = a + 0
dt f (t ), find the solution f (t). Take the Laplace transform to obtain
a F (s) a
F (s) = + or F (s) = ,
s s s−1
from which f (t) = a et .
Differentiation:
df (t)
L = s L[f (t)] − f (0) = s F (s) − f (0). (22.10)
dt

Example: Given df (t)/dt − af (t) = c with f (0) = 0, find f (t). Taking the Laplace transform gives
c c c/a c/a
sF (s) − f (0) − aF (s) = or F (s) = =− +
s s(s − a) s s−a
Inversion of this result gives the solution f (t) = (c/a)[−1 + eat ].
Higher Order Derivatives:

dn f (t) n
L = s n
F (s) − sn−m f (m) (0− ), (22.11)
dtn m=1

where f (n) (0− ) ≡ dn f (t)/dtn |t=0− .


Sec. 22.1. Mathematical Transforms 1159

Convolution:
 t  t
−1
L [F (s)G(s)] = dτ f (t − τ )g(τ ) = dτ f (τ )g(t − τ ) (22.12)
0 0

Example: Given F (s) = ω/[s(s2 + ω 2 )], find f (t). If one lets G(s) = 1/s and F (s) = ω/(s2 + ω 2 ), then
g(t) = 1 and f (t) = sin ωt. From this theorem, one then has
 t  t
1
f (t) = dτ g(t − τ )f (τ ) = dτ sin ωτ = (1 − cos ωt).
0 0 ω
Shift Formula:
"
−1 −as f (t − a), t≥a
L [e F (s)] = (22.13)
0, t<a

Example: Given F (s) = e−2s /(s + 1), what is f (t)? Recall that if G(s) = 1/(s + 1) then g(t) = e−t . By this
theorem, one then has " −(t−2)
e , t≥2
f (t) =
0, t<2
Translation Formula:
L[e−at f (t)] = F (s + a) (22.14)

Example: Given F (s) = s/[(s + a)2 + ω 2 ], find f (t). One can rewrite F (s) as
(s + a) − a
F (s) = ≡ G(s + a)
(s + a)2 + ω 2
where
s a a
G(s) = − 2 for which g(t) = cos ωt − sin ωt
s2 + ω 2 s + ω2 ω
Then from this theorem, f (t) = e−at (cos ωt − ωa sin ωt).
Initial Value Theorem:
lim|s|→∞ [sF (s)] = limt→0 f (t) (22.15)

Example: If F (s) = s/(s2 + ω 2 ), what is f (0)? From tables one knows f (t) = cos ωt so that f (0) = 1. We
can get this same result from the theorem, namely,
s
f (0) = lim s = 1.
|s|→∞ s2 + ω 2
Final Value Theorem:
lim|s|→0 [sF (s)] = limt→∞ f (t) (22.16)

Example: If F (s) = 1/[s(s + 2)], what is limt→∞ f (t)? From tables one finds f (t) = (1 − e−2t )/2 so that
f (∞) = 1/2. From this theorem, the same result is obtained, namely
1 1
f (∞) = lim s = .
|s|→0 s(s + 2) 2
1160 Nuclear Electronics Chap. 22

22.1.4 The Transfer Function


The dynamic response (output) y(t) of a linear network of components to an input x(t) is generally described
by a set of linear coupled differential equations. By taking the Fourier or Laplace transforms of these dynamic
equations, they are transformed into a set of algebraic equations involving the transforms X(s) and Y (s) (or
X(ω) and Y (ω)).
The transfer function describes the ratio of two signals, usually the signal output of a circuit divided
by a corresponding input signal. Denoting x(t) as the time dependent input signal and y(t) as the time
dependent output signal, then the Fourier transfer function is
Y (ω) F (y(t))
T (ω) = = , (22.17)
X(ω) F (x(t))
and the Laplace transfer function is
Y (s) L(y(t))
H(s) ≡
= . (22.18)
X(s) L(x(t))
For the Laplace transfer function, it is usual to assume the initial values x(0) and y(0) are both zero.
Values that cause the numerator of Eq. (22.18) to become zero are called zeros, and values that cause the
denominator to become zero are poles. The poles of the transfer function play a key role in the behavior of
y(t) when Y (s) is transformed back into the time domain. This behavior and the importance of poles are
discussed later in the chapter. A hint of the importance of poles can be seen from the entries in Table 22.1
where the poles in F (s) determine the time and scaling constants in f (t).
Often a dynamic system (here a circuit) is considered that is in steady-state for t < 0 and then for t ≥ 0
some time-dependent input x(t) (or deviation from the steady-state input) is applied to the system so as to
produce an output y(t) (or deviation from its steady-state output). The output y(t) could be obtained by
solving the differential equations describing the dynamic behavior of the system. However, the same solution
can be obtained from the transfer function of Eq. (22.18) as
y(t) = L−1 [X(s)H(s)]. (22.19)
−1
In particular, if x(t) = δ(t) the output h(t) produced by this unit impulse input is h(t) = L H(s) since
X(s) = L[δ(t)] = 1. Once the impulse response is known, the output y(t) for any input x(t) can be obtained
with the convolution property of Laplace transforms as
 ∞
y(t) = L−1 [H(s)Y (s)] = h(τ )x(t − τ ) dτ. (22.20)
0

The frequency response of electric circuits is important in characterizing the circuit. This response can
also be obtained directly from the transfer function. If the input for t ≥ 0 is x(t) = xo sin ωt the output can
be shown to be2
y(t) = xo |H(jω)| sin(ωt + φ) + decaying transient terms. (22.21)
Thus, a sinusoidal input produces, asymptotically, a sinusoidal output with a phase shift φ. The gain G(ω)
of the circuit is the ratio of the amplitude of the asymptotic sinusoidal output to that of the input, i.e.,
G(ω) = |H(jω)|, (22.22)
and the phase shift φ(ω) is
ImH(jω)
φ(ω) = argH(jω) = tan−1 . (22.23)
ReH(jω)

2 If H(s) has a pole at s = 0, then a constant shift also appears in the right-hand side of Eq. (22.21).
Sec. 22.2. Pulse Shaping 1161

Example 22.2: What are the zeros and poles of the transfer function?
s(s + 3)
H(s) = .
(s − 2)(4 + s)2

Solution:
This transfer function has simple zeros at s = 0 and s = −3. It also has a pole of order 1 at s = 2 and a
pole of order 2 at s = −4.

22.2 Pulse Shaping


The production of induced charge in a radiation detector was described earlier in Chapter 8 where it was
seen that the amount of charge created is linearly proportional to the energy deposited by a radiation event
in the detector. Signals from a radiation detector usually develop rapidly and are of short duration, mainly
because the charge induction continues only while the free charge carriers are in motion inside the detector
medium. The goal of a detection system is to measure accurately the charge produced in a detector and to
generate an output signal that corresponds linearly to the liberated charge. The method used to measure
this charge involves pulse shaping, wherein the input current from the detector is changed to an output
voltage pulse with a maximum that is proportional to the initial charge liberated in the detector.
Imperfections with the pulse processing electronics
often introduce artifacts into the output stream of pulses v(t) v(t)
as a result of pulse pile-up, ballistic deficit, and electronic V0 V0
noise. Radiation induced pulses arriving at the input of
the processing electronics are stochastic, meaning that t t
they arrive at random times. Consider the pulse train 0 0
shown in Fig. 22.1 generated from monoenergetic ra- (a) (b)
diation interactions. The ideal situation would be to Figure 22.1. The effects of pulse pile-up for (a) tail pulses
have the processed pulses all have identical heights for with relatively long tails and (b) tail pulses with long un-
identical energies. However, in the case depicted by dershoot. The pulse height without distortions is v0 .
Fig. 22.1(a), voltage pulses arrive before the electronic tail of previous pulses have relaxed to zero, ef-
fectively causing them to appear larger than they really are. In the case depicted by Fig. 22.1(b), the pulse
tails have long undershoots, i.e., they extend to negative values before the electronics reset. Consequently,
some pulses appear to be smaller than they actually are. Both of these cases are caused by pulse pile-up in
which radiation events occur faster than the electronics can respond. Both cases can cause serious deleterious
effects on radiation spectroscopy by widening the pulse height spectrum.
The term “ballistic” deficit refers to the situation in which the output pulses have a lower output ampli-
tude than expected because the processing electronics prematurely ends the signal formation. Unfortunately,
this premature pulse termination is often necessary to increase the pulse processing speed in order to accom-
modate high rates of radiation interactions. Under ideal conditions, the ballistic deficit would be proportional
to the amount of induced charge and have little effect on spectroscopic performance. However, gas-filled and
semiconductor detectors have induced currents that vary with the trajectory of an ionizing particle and with
the interaction location. This effect, thus, broadens the energy resolution of the spectrometer.
Electronic noise produces a variation among ideally identical radiation-induced signals and, thus, causes
broadening in the energy resolution of a spectrometer. The average noise voltage should be zero with
some standard deviation about zero, or about the root mean square (RMS) voltage. Input pulses have the
1162 Nuclear Electronics Chap. 22

randomized noise added, positively or negatively, to the signal so that the energy resolution is broadened.
Noise is most problematic in the early stages of amplification. Sources of noise and mitigation methods are
discussed in a latter section of this chapter.

22.2.1 Circuit Element Impedances


R C L There are three main passive elements used in electronic circuits, namely
resistors, capacitors, and inductors. The resistor is a passive element
+ - + - + -
i i(t) di(t)/dt
that, as the name implies, resists the flow of electrical current in accor-
dance with Ohm’s law
(a) (b) (c)
dq(t)
Figure 22.2. Symbols for passive cir- v(t) = i(t)R = R , (22.24)
cuit elements, (a) resistor, (b) capaci-
dt
tor, (c) inductor. where v(t) is the voltage, i(t) is the current, q(t) is the charge, and R is
the resistance with units of ohms (Ω).3 The symbol for a resistor is a zig-zag line as depicted in Fig. 22.2(a).
A capacitor is a passive device in which two conductors are separated by an insulator (see Sec. 8.3)
capable of storing charge when a voltage is applied across the terminals. Capacitance C is the ratio of stored
charge q(t) to the resulting voltage v(t) (charge per volts) and has units of farads (F ), or ampere-second per
volt. Thus
q(t)
v(t) = . (22.25)
C
If the stored charge changes with time, then the resulting current is
dq(t) dv(t)
i(t) = =C . (22.26)
dt dt
An inductor produces a magnetic field when a current flows through it. Further, if the current flowing
into the inductor changes with time, an induced voltage is produced that is proportional to the rate of
change, namely,
di(t) d2 q(t)
v(t) = L =L , (22.27)
dt dt2
where the inductance L is the ratio of change between the induced voltage and the change in current and
has units of henries (H), or volt-second per ampere.
Phasors and Impedances
If a circuit contains capacitors and/or inductors, equations for currents and voltages involve time deriva-
tives. So, even for the simplest circuits, transient responses are generally described by ordinary differential
equations. Only for circuits composed solely of resistors are the voltage and current transients given by
simple algebraic equations. However, there is one important case where the differential equations can be
replaced by algebraic equations, namely when the voltages and currents are sinusoidal functions of time.4
To obtain such a simplification, it is necessary to use the complex plane and introduce complex quantities
such as phasors and impedances.
Sinusoidal voltages and currents can always be written as

v(t) = vo sin(ωt + φv ) and i(t) = io sin(ωt + φi ), (22.28)

3 Here lowercase v, q, and i are used to denote generally time-dependent quantities, whereas their uppercase counterparts, used
for example in Chapter 8, generally denote steady-state values.
4 The same simplification is obtained with the more complex Laplace transform technique, which is applicable to any type of

transient. But the special case of sinusoidal transients is a well-established fixture of circuit analysis.
Sec. 22.2. Pulse Shaping 1163

where vo and io are amplitudes, φv and φi are the phase shifts, and ω is the angular frequency. Any complex
number z can be written in terms of its real and imaginary parts as {z} + j{z}. Then with Euler’s
theorem ejωt = cos ωt + j sin ωt, the real parts of v(t) and i(t) can be written as

v(t) = {vo ej(ωt+φv ) } = {vejωt } and i(t) = {io ej(ωt+φi ) } = {iejωt },

where the complex numbers v ≡ vo ejφv and i ≡ io ejφi are often called phasors. Note that the phasors are
independent of time. Then the derivatives of the voltage and current can be written as

dv(t) di(t)
= {jωvejωt } and = {jωiejωt }. (22.29)
dt dt
Hence, in the complex plane, differentiation with respect to t is the same as multiplication by jω. In this
manner, the differential equations for the analysis of a circuit are converted into algebraic equations. The only
difference is that currents and voltages are now phasors and the resistances, capacitances and inductances
are replaced by their complex impedances defined as the phasor ratio v/i with units of ohms (Ω).
As an example of an impedance, consider a sinusoidal voltage placed across a capacitor. The complex
voltage and current are vejωt and iejωt , respectively. Then from Eq. (22.26)

d : jωt ;
iejωt = C ve or i = jωCv.
dt
The capacitor impedance is thus
v 1
ZC = = . (22.30)
i jωC
Equation (22.30) is worth a closer look. At low frequencies, when ω ≈ 0, Eq. (22.30) becomes extremely
large, i.e., the impedance becomes infinite or equivalent to an open circuit. At high frequencies Eq. (22.30)
approaches zero, and the capacitor behaves as a short circuit. The impedances of resistors and inductors
can be found in a similar fashion to give,5

v v 1 v
= ZR = R, (resistor), = ZC = (capacitor), = ZL = jωL (inductor). (22.31)
i i jωC i

Note that the impedances of capacitors and inductors change with signal frequency, and lumped circuits
must include the complex algebraic manipulations of these terms. Further, opposite of the capacitor, the
inductor has high impedance at high frequency and behaves as a short circuit at low frequency. The resistor
has no frequency dependence.
Combining Circuit Elements
The impedances of these elements of resistance, capacitance, and inductance generally follow the rules of
series and parallel resistive circuits, that is, impedances in series

Zeq = Z1 + Z2 + Z3 + . . . + ZN , (22.32)

and impedances in parallel


1 1 1 1 1
= + + + ... + , (22.33)
Zeq Z1 Z2 Z3 ZN

5 The Laplace transform representations are ZC = 1/(sC) and ZL = sL, which are also their transfer functions.
1164 Nuclear Electronics Chap. 22

where the complex terms remain appropriately separated. The real portion of the impedance is called
resistance R (or active component), while the imaginary part is called the reactance X. The magnitude of
a complex impedance is
 
|Z| = |R + jX| = (R + jX)(R − jX) = R2 + X 2 . (22.34)
The phase angle of a complex circuit is  
X
θ = arctan , (22.35)
R
denoted ∠θ relative to 0◦ , that is, positive for leading angle and negative for lagging angle with respect to
the voltage versus current. Consequently, a purely inductive circuit has voltage phase angle of 90◦ leading
the current, while a purely capacitive circuit has voltage phase angle of −90◦ lagging the current.

Example 22.3: Find the impedance of the following circuit:


C

R
L
Solution:
First, the parallel combination of the impedance is
 
1
−1 (jωL)
1 1 Z1 Z2 jωC jωL
Z = + = = =
Z1 Z2 Z1 + Z2 1 1 − ω 2 LC
jωL +
jωC
Now add the series resistance to find
jωL R(1 − ω 2 LC) + jωL
Zeq = R + = .
1 − ω LC
2 1 − ω 2 LC
The magnitude is <  2
ωL
Zeq = R2 + ,
1 − ω 2 LC
with phase angle
ωL
θ= ,
R(1 − ω 2 LC)
which, at low frequency (ω 2 LC 1), becomes
ωL
θ≈ ,
R
and at high frequency (ω 2 LC  1)
−1
θ≈ .
ωRC
What then does this mean? The phase angle is zero for DC voltage applied to the circuit. At low
frequencies, the phase angle is positive, and at high frequencies the phase angle is negative. A resonant
frequency appears at ωo2 = 1/LC, meaning that the magnitude of the impedance effectively becomes infinite,
behaving as a notch (or band-stop) filter at the resonant frequency.
Sec. 22.2. Pulse Shaping 1165
4

1 v1 + 1
i1 = 0
A(v2-v1)
A 3 +
3
2 + v2 + 2 +
i2 = 0
5
(a) (b)
Figure 22.3. Usual depiction of an operational amplifier showing the basic inputs
1 and 2 and output terminal 3. Power is provided at terminals 4 and/or 5.

22.2.2 Operational Amplifier


A basic building block of a preamplifier is often the operational amplifier (or “op amp”), usually depicted as
a right pointing triangle with two inputs and one output. This simplistic figure takes the place of a complex
network of transistors, resistors, and capacitors that generally make up the actual op amp [Irvine 1981]. For
instance, the common 741 op amp has three amplification stages and 20 or so transistors.
The operational amplifier has two input terminals, identified as 1 and 2 in Fig. 22.3(a), and one output
terminal, denoted as terminal 3. The devices require power to operate, usually applied at terminal 4 (positive)
and 5 (negative). A common operating voltage requirement is ±9 volts, although modern amplifiers may
operate on only a few volts. The open-loop gain is denoted by A, which is typically very large usually between
105 to 107 for constant input voltages. An op amp may also have additional terminals designated for special
purposes, such as frequency compensation and offset nulling.
The main function of an op amp is to sense the difference between the voltage inputs at terminals 1
(v1 ) and 2 (v2 ), each referenced to ground, and supply amplification A(v2 − v1 ) at terminal 3. For low
frequency inputs, the open-loop gain A has a large value. But at some breakpoint frequency the gain begins
to decrease with frequency at -20 db/decade, and where the open-loop gain crosses 0 db is defined as the
open-loop bandwidth. The closed-loop bandwidth of an op amp is the frequency range over which the gain
remains above -3 db of its value at ω = 0. The frequency dependence of the open-loop gain, as discussed
in the next sections, is important as it is a major contributor to the non-ideal performance of an op amp
circuit. Detailed analysis for op amp performance can be found in a number of references, including Carter
and Brown [2016], Carter and Mancini [2017], Jung [2005], and Zumbahlen [2008].
Ideally, an op amp should have an infinite input impedance, thereby eliminating input current. Further,
the output impedance at terminal 3 should be zero, such that there is no voltage loss from the ideal gain
A(v2 − v1 ). The equivalent circuit is shown in Fig. 22.3(b). Terminal 1 is called the inverting terminal, and
terminal 2 is the non-inverting terminal.
Consider the situation of Fig. 22.3(b). If the output at terminal 3 is in fact A(v2 − v1 ), then the following
applies for the output voltage at terminal 3
v3
= (v2 − v1 ). (22.36)
A
Because A is large, and ideally treated as infinite, then it is found that
v3
= (v2 − v1 )  0. (22.37)
A
Consequently, if A is very large, and approaching infinity as in the ideal case, then v1  v2 , a condition
emulating a short circuit between terminals 1 and 2. For this reason, there is a virtual short circuit between
1166 Nuclear Electronics Chap. 22

terminals 1 and 2. Also, if terminal 2 is connected to ground, then terminal 1 is effectively also connected
to ground through the virtual short circuit, and is referred to as a virtual ground.

22.2.3 The General Case for Feedback Transfer Function


Consider the op amp configuration of Fig. 22.4(a). There is an input
voltage applied across an impedance into the inverting input. Also,
-vout /A another impedance is placed across the inverting input terminal and
Z2
the output terminal. With the positive terminal grounded, the voltage
i1 i2
iin = 0 at the inverting terminal must be vin = −vout /A.
Z1
+ The current i1 is defined as
+ 0V A
vin (−vout /A) − vin 1 vout
+ + i1 = =− vin + . (22.38)
vout Z1 Z1 A
Because of the high input impedance at the inverting input, the cur-
(a)
rent across the feedback impedance Z2 is practically the same as that
vin
vB + across the impedance Z1 (i2 ≈ i1 ). The output voltage vout must be
+ + the sum of the voltages at the inverting input terminal and across Z2
vAB A vout 1 vout
+ vout = − − vin + Z2 (22.39)
vA vout A Z1 A
Rearranging terms yields
Z1 Z2
i1 i2 vout Z2 1
=− . (22.40)
vin Z1 1 + (1 + Z2 /Z1 )/A
(b)
Figure 22.4. The (a) inverting configura-
Recalling that the value of A is large, Eq. (22.40) reduces to
tion and the (b) non-inverting configuration
vout Z2
with generalized impedances. ≈− . (22.41)
vin Z1
Hence, the transfer function for Fig. 22.4(a) is

Z2 (s)
H(s) = − . (22.42)
Z1 (s)

A similar analysis can be used to show that the non-inverting case of Fig. 22.4(b) results in the following:

vout Z2 Z1 (s) + Z2 (s)


≈1+ , with H(s) = . (22.43)
vin Z1 Z1 (s)

22.2.4 Passive Low-Pass Filter


A simple low-pass filter is depicted in Fig. 22.5, in which a time dependent input voltage vin (t) is placed
across the resistor and the capacitor. As a result the voltage vout (t) is formed across the capacitor and is
measured as a function of time. From the figure the voltage across the resistor must equal the difference
between the input voltage and the voltage across the capacitor, i.e.,

vin (t) − vout (t) = Riin (t). (22.44)


Sec. 22.2. Pulse Shaping 1167

iin vin(t) vout(t)


The current flowing to the capacitor is
R
vin C vout
dQ(t) dvout (t)
iin (t) = =C , (22.45) t
t
t
dt dt (a)
0
(b)
0
(c)

where Q(t) = Cvout (t) is the charge accumulated on the ca- Figure 22.5. The (a) basic low-pass circuit and
pacitor as a function of time. Substitution of Eq. (22.45) into result from a (b) step function input vin (t) with
Eq. (22.44) and rearrangement gives (c) output response vout (t).

dvout (t) 1 1
+ vout (t) = vin (t), (22.46)
dt τ τ
where τ = RC is the time constant. The most general solution of this linear, first-order, ordinary differential
equation is
 t
−t/τ −  vin (t )
vout (t) = e vin (0 ) + et /τ dt , (22.47)
0 τ
where vin (0− ) is the initial voltage condition. Often it is assumed that vin (0− ) = 0 for many solutions.

Step Input
For Vin (0− ) = 0, or no initial charge, and for the step input shown in Fig. 22.5(b) with vin (t) = vin
o
for t > 0,
this general solution reduces to
o
vout (t) = vin 1 − e−t/τ , t ≥ 0. (22.48)
o
Consequently, the output signal is an increasing exponential function that approaches the input voltage vin .
Note that the rate of increase is a function of the time constant, which can be altered by changing either C, R,
or both. The smaller the time constant, the faster the rise to vin . Depicted in Fig. 22.5(c) is the response to
a voltage step input, where the tangent of the initial signal rise intersects the maximum possible output value
at t = τ . Stated differently, the difference between vout (∞) and vout (τ ) equals vout (∞)/e  0.368vout (∞).

Oscillatory Input
To determine the frequency characteristics of this device, first take the Laplace transform of Eq. (22.46) and
rearrange to obtain the transfer function

1 1
H(s) = = . (22.49)
1 + sRC 1 + sτ

The voltage gain, defined here by Eq. (22.22), is


    
 1  1 1
1/2
1 1

G(ω) = |H(jω)| =   = = =√ , (22.50)
1 + jωτ  1 + jωRC 1 − jωRC 1 + (ωRC)2 1 + ω2τ 2

which at low frequencies is G(ω)  1, i.e., the amplitude of the output sine wave equals that of the input
sine wave. But at high frequencies G(ω)  1/ωτ and the output amplitude decreases as 1/ω. Because low
frequencies of the input pass, without change, to the output while high frequencies are attenuated, the circuit
of Fig. 22.5 is called a low-pass filter. The cut-off frequency is given by

1 1 1 1
fc = = or 2πfc = ωo = = . (22.51)
2πRC 2πτ RC τ
1168 Nuclear Electronics Chap. 22

The voltage gain is often expressed in decibels6 as


Gdb (ω) = 20 log10 |H(jω)|. (22.52)
The phase shift is  
ImH(jω)
φ(ω) = tan−1 = − tan−1 (ωτ ) . (22.53)
ReH(jω)
At the frequency ω = 1/τ , then φ = −45◦ .

Example 22.4: Given R = 1 MΩ and C = 10 pF, what is the cutoff frequency of the low-pass filter?

Solution:
1 1
fc = = = 15.916 kHz.
2πCR 2π(106 Ω)(10−11 F)
So the cutoff frequency is 15.916 kHz. To test this result wc = 2πfc so
 
1 1
|Gdb (ω)| = 20 log10  = 20 log10 √ = −3 dB,
1 + (ωo RC)2 2
Hence, at the cutoff frequency, the output magnitude has dropped by 3 dB.

22.2.5 Active Low-Pass Filter


Two simple active low-pass filters (inverting config- C 2
summing summing
urations) are depicted in Fig. 22.6. In the case depicted junction
C
junction
2
i i R
by Fig. 22.6(a) v 1 1
A v 1 1
A
2

vin (t) R + 1 R + 1
i1 (t) = . (22.54) +v v A 3 AB
+
v
v A 3 AB
R1 +in +
+ + in

v 2 v B v 2 outv B out
If the initial condition has the voltage across the feed-
back capacitor C2 of V0 then (a) (b)
 t  t Figure 22.6. Simple low-pass amplification circuits de-
1 1
vout (t) = V0 − i1 (t) dt = V0 − vin (t) dt. picting the (a) ideal integrator and the (b) practical inte-
C2 0 R1 C2 0 grator.
(22.55)

6 The decibel is actually a logarithmic measure of the ratio of power output to input. The power gain is
 v2 /Zout
 Pout
G = = out2 /Z
power Pin vin in

where P = v2 /Z. Expressed in decibels,


  2   
 vout Zout
Gdb (ω) = 10 log10 2
− 10 log10 .
power vin Zin
Note that if Zin = Zout , then power gain and voltage gain are equivalent when expressed in decibels
 
 
Gdb (ω) = 10 log10 |H(jω)|2 = 20 log10 (|H(jω)|) = Gdb (ω) .
power voltage
Sec. 22.2. Pulse Shaping 1169

Hence, the output is the integral of the input and, thus, the reason this circuit is called an integrator.
Also, R1 C2 is the integration time constant. The negative output is a consequence of the inverting op amp
configuration. If the input is taken as vin (t)− V0 so as to give a zero initial condition, the closed loop transfer
function is
1
Z2 (s) sC −1
H(s) = − =− 2 = , (22.56)
Z1 (s) R1 sR1 C2
which has gain
1
G(ω) = |H(jω)| = . (22.57)
ωR1 C2
A positive voltage input produces a negative output, while a negative input produces a positive output.
The output voltage remains constant if there is a zero value input. Suppose a series of positive square pulses
is applied to the input. With the ideal integrator, every positive pulse produces a progressively increasing
negative voltage on the output. This sequential increase occurs because the feedback capacitor C2 does
not discharge, but instead continues to accumulate charge for every pulse. However, this simple integrating
circuit has several drawbacks. Eventually the integrator circuit saturates, and the circuit no longer responds
to input voltages until the capacitor is discharged. The saturation is a result of a small difference in voltage
across the input terminals due to slight transistor mismatching in the amplifier circuit. Over time, this small
offset voltage continues to accumulate on the capacitor until, eventually, it changes the baseline V0 enough
to distort the output signal or to saturate the preamplifier. Another difficulty arises because the bandwidth
of an ideal integrator is small so that it can be used over only a small input range of frequencies.
These problems can be remedied by placing a feedback resistor R2 in parallel with C2 , as shown in
Fig. 22.6(b), a design traditionally labeled the practical integrator. The transfer function for this arrangement
is
−1
1
+ sC2  
Z2 (s) R2 R2 1
H(s) = = = (22.58)
Z1 (s) R1 R1 (1 + sR2 C2 )
with gain
  1/2
R2 1
|G(ω)| = . (22.59)
R1 (1 + (ωR2 C2 )2
At low frequency, the gain is R2 /R1 , and the angular cutoff frequency is
1
ωo = 2πfc = . (22.60)
R2 C2
Also with this integrator configuration, capacitor C2 now discharges with time constant τ = R2 C2 .

22.2.6 Passive High-Pass Filter


A simple passive high-pass filter is depicted in vin(t) vout(t)
Fig. 22.7, in which a time-dependent input voltage vin (t) C

is placed across the capacitor and the resistor so that a vin R vout
voltage vout (t) is formed across the resistor. The dif-
0 t 0 t t
ference between the input and output voltages is the (a) (b) (c)
voltage Q/C developed across the capacitor C, i.e.,
Figure 22.7. The (a) basic high-pass circuit and result
Q(t) from a (b) step function input vin (t) with (c) output re-
vin (t) − vout (t) = . sponse vout (t).
C
1170 Nuclear Electronics Chap. 22

Differentiation with respect to time gives

dvin dvout (t) 1 dQ(t)


− = . (22.61)
dt dt C dt
But i(t) = dQ/dt = vout (t)/R and, with τ = RC, Eq. (22.61) becomes

dvin (t) dvout (t) vout (t)


= + . (22.62)
dt dt τ
Take the Laplace transform of Eq. (22.62) to obtain the transfer function

sRC sτ
H(s) = = . (22.63)
1 + sRC 1 + sτ
The gain of this circuit is then
  <
  
 vout (t)  jωRC −jωRC
1/2
ω 2 R2 C 2

|G(ω)| =   = = . (22.64)
vin (t)  1 + jωRC 1 − jωRC 1 + ω 2 R2 C 2

From Eq. (22.64), it is seen that at high frequencies G(ω)  1, i.e., vout ≈ vin . By contrast, at low
frequencies ω  1 G(ω)  ω so vout decreases as ω decreases. Thus, the name high-pass filter for this device.
The low-frequency cutoff is also
1
2πfc = ωo = ,
RC
where |G(ωo )| = −3 dB.
Step Input to Passive High-Pass Filter
Given a positive step input of height vin (t = 0), as depicted in Fig. 22.7(b), there is an instantaneous change
o
in vin at t = 0. Otherwise, the input voltage remains constant at vin . Thus Eq. (22.62) becomes

dvin (t) dvout (t) vout (t)


=0= + , (22.65)
dt dt τ
which, upon integration, gives
o −t/τ
vout (t) = vin e , t > 0. (22.66)
Thus, a step input produces a tail pulse with a decay constant τ = RC.
Rectangular Pulse Input to a Passive High-Pass Filter
o
If a square wave pulse input vin (t) with width tp and height vin is applied to the passive high-pass filter at
t = 0, the initial response is the same as the step input. However, at the end of the pulse, the input voltage
returns to zero. However, the voltage across the capacitor in the circuit cannot immediately return to zero
because the discharge current is limited by the resistor. Consequently, the output must decrease by the pulse
o
input vin , or,
o −tp /τ
vout (tp ) = vin e − vin
o
, (22.67)
which shows that the output becomes negative. Beyond tp , the pulse exponentially decays back to zero as

o
vout (t) = vin e−tp /τ − 1 e−(t−tp )/τ , t ≥ tp . (22.68)
Sec. 22.2. Pulse Shaping 1171

To explore the consequences of this result, consider the cases where τ tp and τ  tp . If τ tp , then the
output pulse has decayed very little at time tp so that the negative undershoot is very small and has little
effect on the output. If instead τ  tp , then much decay occurs well before tp is reached so that the positive
o
output voltage spike and the negative undershoot has the same magnitude as vin and appears as a negative
spike. Another less obvious result can be found by integrating and comparing both Eqs. (22.66) and (22.68)
within their respective operating times, namely
 tp
o −t/τ

o −t/τ tp
vin e = −τ vin e 0
o
= τ vin 1 − e−tp /τ
0

and
 ∞
∞ 
o
vin e −tp /τ
−1 e −(t−tp )/τ
= o
vin 1−e tp /τ
−τ e −t/τ  = −τ vin
o
1 − e−tp /τ . (22.69)

tp tp

Hence, the area under the output pulse before tp and then after tp are equal (with opposites signs). Conse-
quently, the time it takes to return to zero can be unacceptably long if the circuit has large τ .
Series of Rectangular Pulses to a Passive High-Pass Filter
The natural extension of the analysis for the input of a single rectangular pulse is to consider a series of
rectangular pulses. Suppose that the input voltage is a rectangular pulse of duration t1 and constant voltage
v1 followed by a lower constant voltage v2 of duration t2 . The total period of a cycle is, therefore, T = t1 + t2
with a total voltage swing of V = v1 − (−v2 ) = v1 + v2 . This voltage swing can be displaced by a DC voltage
shift vDC as shown in Fig. 22.8(a). In other words, the actual high-input voltage is v1 + VDC and the actual
low-input voltage is VDC − v2 .
Because the output voltage vout (t) is unaffected by VDC (a high-pass filter does not pass a constant
voltage), for the following analyses one can assume any value of VDC . If one chooses VDC = −v2 then
Eq. (22.61) for vout (t) can be written as
dvout (t) 1 dvin (t)
+ vout (t) = , (22.70)
dt τ dt
where the input wave form for cycle n is
$
v1 − v2 ≡ vin
o
(n − 1)T ≤ t < (n − 1)T + t1
vin (t) = . (22.71)
v2 − v2 = 0 (n − 1)T + t1 ≤ t < nT
The solution of Eq. (22.70) for any vin (t) is
 t
 dvin (t ) 
vout (t) = e−t/τ vout (t−
o)+ et /τ dt , t > to , (22.72)
t−
o
dt
where t−o is the time just before the start of transient calculation.
o
The output voltage during any cycle has two parts: (1) that during the rectangular pulse when vi (t) = vin
and (2) that during the time when vin (t) = 0. For the first portion to is the time the pulse begins, and for
the second portion to is the time the pulse ends. The transients for both portions can be calculated from
Eq. (22.72) using the appropriate value of vin (t− o ). Because vin (t) consists of two step functions, dvin /dt
consists of two delta functions since the derivative of a step function is a delta function. In particular, for
the nth cycle
dvin (t) o
= vin δ(t − [n − 1]T )) − vin
o
δ(t − [n − 1]T − t1 ). (22.73)
dt
The output voltage is now calculated cycle by cycle.
1172 Nuclear Electronics Chap. 22

vin T
vout
t1 t2 T t T
t1 t2
v1
vavg vino A1 v1 vino
vDC v2 0
0 A2 v2 t
(a)
t (b)
vout T vout
t1 t2 t T T t T
t1 t2
vino
vino vino v1min v1max
0 0
vino t v2min t
v2max
(c) (d)
Figure 22.8. (a) Square wave input with a DC offset, (b) output from a passive
differentiator circuit with τ  T , (c) output from a passive differentiator circuit with
τ  T , (d) output from a passive differentiator circuit with τ > T . Shown in the output
voltage plots are the voltages obtained after a large number of cycles, i.e., when each
cycle has the same response.

Cycle 1 (0 < t < T ): For the first portion of this cycle, to = 0, vin (t− o
o ) = 0 and dvin /dt = vin δ(t).
Substitution into Eq. (22.72) gives
o −t/τ
vout (t) = vin e , 0 ≤ t < t1 . (22.74)
For the second portion of this cycle, to = t1 and dvin /dt = −vin
− t1 ). Then from Eq. (22.72) one finds
o
δ(t
 
vout (t) = −vin
o
1 − e−t1 /τ e−(t−t1 )/τ , t1 ≤ t < T. (22.75)

More compactly the response in the first cycle can be written as


$
vout (t) e−t/τ , 0 ≤ t < t1
o = −(t−t1 )/τ
, (22.76)
vin −βe , t1 ≤ t < T
where β ≡ 1 − e−t1 /τ < 1.
Cycle 2 (T < t < 2T ): For the first portion of this cycle to = T , vout (t− o ) = −vin βe
o −(T −t1 )/τ
, and
dvin /dt = vin δ(t − T ). For the second portion of the cycle, to = T + t1 , vin (to ) equals the final voltage of the
o

first portion, and dvin /dt = −vin o


δ(t − T − t1 ). Expressions for the transients in both portions of the cycle
are obtained from Eq. (22.72).
$
vout (t) [α + e−T /τ ]e−(t−T )/τ , T ≤ t < T + t1
o = −T −(t−T −t
, (22.77)
vin −[β + βe /τ
]e 1 )/τ
, T + t1 ≤ t < 2T
where α ≡ 1 − e−t2 /τ < 1.
Sec. 22.2. Pulse Shaping 1173

Cycle n ((n − 1)T < t < nT ): One can continue in this fashion cycle after cycle to obtain vin (t) in each
successive cycle. By induction, the response for the nth cycle, which begins at t = tn−1 ≡ (n − 1)T , is
⎧  n−1 
⎪ α  e−(k−1)T /τ + e−(n−1)T /τ e−(t−(n−1)T )/τ , t


⎪ n−1 ≤ t < tn−1 + t1
vout (t) ⎨
= k=1  . (22.78)
o
vin ⎪
⎪ n

⎪ −(k−1)T /τ −(t−(n−1)T −t
⎩ − β tn−1 + t1 ≤ t < nT
1 )/τ
e e ,
k=1

Large n: The sums in Eq. (22.78) are a geometric progression



n
1 − γ n−1
Sn = e−(k−1)T /τ = 1 + γ + γ 2 + . . . γ n−1 = , (22.79)
1−γ
k=1

where γ ≡ e−T /τ < 1. As n → ∞, Sn → 1/(1 − γ) and from Eq. (22.78), in the limit of large n,
⎧ α

⎪ e−t/τ , 0 ≤ t < t1
vout (t) ⎨ 1 − γ
= , (22.80)
o
vin ⎪
⎪ −β −(t−t1 )/τ
⎩ e , t1 ≤ t < T
1−γ
where t is now measured from the start of a cycle.
The area A1 under vin (t) during the rectangular pulse is
 t1
α v o ατ v o αβτ
A1 = vino
e−t/τ dt = in (1 − e−t1 /τ ) = in . (22.81)
1−γ 0 1−γ 1−γ
Likewise the area A2 under vin (t) between t1 and t1 + t2 is

β t1 /τ t1 +t2 −t/τ v o βτ v o αβτ
A2 = −vin
o
e e dt = − in (1 − e−t2 /τ ) = − in . (22.82)
1−γ t1 1−γ 1−γ
Thus, it is seen that A1 = −A2 , i.e., the two shaded areas in Fig. 22.8 are equal. This equality of the areas
for the positive and negative transients is true only for the equilibrium cycle (n → ∞) of Eq. (22.80). For
the cycles building up to the equilibrium cycle, A1 > −A2 .
Effect of the Time Constant τ The output response is greatly influenced by the circuit time constant τ .
Regardless of the average input voltage (the DC offset), the output signal is averaged about zero (no DC
component). For an equilibrium cycle (large n), the maximum positive output from Eq. (22.80) is
α o
v1max = v (22.83)
1 − γ in
and the minimum positive voltage is
α o −t1 /τ
v1min = v e = v1max e−t1 /τ . (22.84)
1 − γ in
At tp1 , the polarity switches by −vio (as it does for all cycles), producing the maximum negative voltage
β
v2max = vo (22.85)
1 − γ in
1174 Nuclear Electronics Chap. 22

The negative voltage decays towards zero and reaches a minimum negative voltage at t = T of
β
v2min = v o e−(t2 −t1 )/τ = |v2max |e−(t2 −t1 )/τ . (22.86)
1 − γ in
Then, as expected,
−t2 /τ −t1 /τ
o α −t1 /τ β o [(1 − e )e + (1 − e−t1 /τ )] o
v1min + v2max = vin e + = vin = vin . (22.87)
1−γ 1−γ 1 − e−(t1 +t2 )/τ
For small τ  T , the output rapidly decays to zero before tp is reached, causing a flip in polarity equal
o
to vin at either t1 (goes negative) or t2 (goes positive). Thus a small time constant produces spike peaks of
equal magnitudes alternating in polarity, as depicted in Fig. 22.8(c). For long τ T , there is hardly any
decay, and the output as a rectangular wave that mimics the input, but one with an average of zero (no DC
component). This case is depicted in Fig. 22.8(b). The expected result for cases between these extremes is
depicted in Fig. 22.8(d).
Exponential Input to Passive High-Pass Filter
Consider an exponential input to a high-pass filter with the form7
o
vin (t) = vin 1 − e−t/τin (22.88)
o
where vin is the maximum voltage reached as t → ∞ and τin is the time constant of the input signal.
Substitution of Eq. (22.88) into Eq. (22.62) gives the differential equation
o
vin dvout vout
e−t/τin = + , (22.89)
τin dt τ
where τ is the time constant RC of the high-pass filter. The solution of this equation is
⎧ τ
⎪ o
⎨ vin τ − τ e−t/τ − e−t/τin , τ = τin
in
vout (t) = . (22.90)

⎩ v o t e−t/τ ,
in τ = τin
τ
Now consider two limiting cases of Eq. (22.90), τ  τin and τ τin . In the former case, one obtains
τ −t/τin
vout (t) ≈ vin
o
e . (22.91)
τin
Here it is seen that as τ decreases with respect to τin , the maximum output pulse height diminishes and
decays according to the input time constant τin . Hence, the condition where τ is much smaller than the time
constant of the input pulse τin causes a ballistic deficit with a ratio τ /τin . For the case in which τ τin ,
Eq. (22.90) reduces to
o −t/τ
vout (t) ≈ vin e . (22.92)
Note that the dependence of vout (t) on τin vanishes and the output depends only on the network decay
o
constant and the maximum output voltage equal to vin . Actual real high-pass networks are somewhere
between the limiting cases of Eqs. (22.91) and (22.92). Generally, the amount of ballistic deficit increases as
τ decreases.
7 Compare this signal input to Eq. (22.48), the output solution of a passive low-pass filter.
Sec. 22.2. Pulse Shaping 1175


 
     




 


 

 

 



 
  
  

        
 
Figure 22.9. Output from a passive high-pass filter from an exponential
input described by Eq. (22.89). Shown are normalized outputs to the
initial input (vout /vin ) as a function of t/τ and τ /τin . The decrease in
the maximum pulse height from unity is the ballistic deficit.

The time to the pulse height maxima is


 
τ τin τ
tmax = ln . (22.93)
τ − τin τin

This result can then be used to calculate the expected maximum in the output pulse height vout (tmax ). The
ballistic deficit is defined as
o
vbd = vin − vout (tmax ). (22.94)
Examples of normalized output pulses with varying time constants are shown in Fig. 22.9. For large values
o
of τ /τin , the pulse height maxima is relatively large and approaches the input value of Vin . However, as τ
decreases, so does the output pulse height maxima, the difference from unity being the ballistic deficit.

22.2.7 Active High-Pass Filter


i2 C2
Simple active high-pass filters (in-
summing summing
verting configuration) are depicted in junction junction
R2
Fig. 22.10. Because terminal 1 is a vir- i1 i1 R2
tual ground, VA = 0 and the output vA 1 vA 1

voltage vout equals the negative of the + +


+ C1
vAB A + R1 C1 vAB A
3 3
voltage across the resistor R2 by the vin + vin +
current i2 , i.e., vB 2
+ vout vB 2
+ vout

vout (t) = v1 (t) = −i2 (t)R2 . (22.95)


(a) (b)
Also because of the high input impe- Figure 22.10. Simple high-pass amplification circuits depicting the (a) ideal
dance at terminal 1, the current flowing differentiator and the (b) practical differentiator.
1176 Nuclear Electronics Chap. 22

to the capacitor C1 must be


dQ dvin (t)
i2 (t) = i1 (t) = = C1 (22.96)
dt dt
Substitution of Eq. (22.95) into Eq. (22.96) yields,
dvin (t)
vout (t) = −R2 C1 . (22.97)
dt
Hence the output vout (t) is the derivative of the input vin (t) so the circuit in Fig. 22.10 is, understandably,
called a differentiator circuit.
The closed-loop transfer function for the circuit in Fig. 22.10(a) is readily obtained by taking the Laplace
transform of Eq. (22.97) to obtain

Vout (s) = −R2 C1 [sVin (s) − vin (0)]. (22.98)


If the initial condition is vin (0) = 0, then the transfer function is simply
Vout (s)
H(s) = = −sR2 C1 with gain G(ω) = |H(jω)| = ωR2 C1 . (22.99)
Vin (s)
The simple differentiator circuit in Fig. 22.10(a) tends to magnify noise and is unstable; hence, this simple
active differentiator circuit is relatively unpopular and seldom used, mainly due to sharp spikes produced at
the output when there is a shape change with the input voltage [Sedra and Smith 1982]. To remedy these
problems, there is an improved version of the differentiator, Fig. 22.10(b) where a resistor R1 has been added
in series with C1 , called the practical differentiator. The transfer function is now
1/2
Z2 −R2 −sR2 C1 (ωR2 C1 )2
H(s) = − = = with gain G(ω) = |H(jω)| = .
Z1 1 1 + sR1 C1 1 + (ωR1 C1 )2
R1 +
sC1
(22.100)
At low frequency, the circuit of Fig. 22.10(b) becomes a high-pass filter, while at high frequency the circuit
becomes an amplifier, with improved noise rejection, with a gain of R2 /R1 . An additional improvement has
a parallel feedback capacitor across R2 , which serves to produce a low-pass filter. Ultimately, the circuit can
perform as a bandpass filter, with transfer function
Z2 −sR2 C1
H(s) = − = . (22.101)
Z1 (1 + sR1 C1 )(1 + sR2 C2 )
From Eq. (22.101), there is a zero at ω = 0, and two poles, one at ω1 = (R1 C1 )−1 (high-pass differentiator
circuit), and one at ω2 = (R2 C2 )−1 (low-pass integrator circuit).

22.2.8 CR-RC Network


The high-pass filters shown in Fig. 22.7 and Fig. 22.10(a) are far iin
A
from ideal and seldom used alone. They produce sharp output C1 R2
peaks that are difficult to process and, because they pass high v R C2 vout
in 1
frequencies they allow high-frequency noise to pass through the
network. These two problems can be effectively mitigated by
adding an integration circuit after the operational amplifier, as
shown in Fig. 22.11. The differentiator and integrator networks
are isolated by the operational amplifier that has a gain of unity Figure 22.11. Depiction of a CR-RC pulse
shaping circuit.
at high frequencies.
Sec. 22.2. Pulse Shaping 1177

In Fig. 22.11 define the time constants τ1 = R1 C1 and τ2 = R2 C2 . Consider the case of a step input
o
vin (t) = vin for t > 0 into this circuit for which vin = vout = 0 for t ≤ 0. The input to the op amp is
described by the output of the high-pass circuit defined by Eq. (22.66), while the output of the low-pass
circuit after the op amp is defined by Eq. (22.46). Let the input to the op amp be vs (t), which is also the
output of the op amp because the gain of the op amp is unity for high frequencies. Then

vs (t) vo dvout (t) vout (t)


= in e−t/τ1 = + . (22.102)
τ2 τ2 dt τ2
Multiply Eq. (22.102) by et/τ2 to find

vs (t)et/τ2 dvout (t) t/τ2 vout (t) t/τ2 d


= e + e = vout (t)et/τ2 . (22.103)
τ2 dt τ2 dt
Substitution of Eq. (22.103) back into Eq. (22.102) leads to

d vo
vout (t)et/τ2 = in et(1/τ2 −1/τ1 ) . (22.104)
dt τ2
Integration of Eq. (22.104) from (0, t) yields
  
vo t
τ1 − τ2
vout (t)e t/τ2
− vout (0) = in exp t dt, (22.105)
τ2 0 τ2 τ1
which, with vout (0) = 0, gives
vout τ1
= e−t/τ1 − e−t/τ2 . (22.106)
vin τ1 − τ2
For the case that τ2 → τ1 Eq. (22.106) becomes indeterminate. But with l’Hôpital’s rule one obtains

d
τ1 (exp[−t/τ1 ] − exp[−t/τ2 ])
vout (t) lim dτ2 t
o =τ2 →τ1 = e−t/τ , (22.107)
vin d τ
(τ1 − τ2 )
dτ2
where τ1 = τ2 = τ . It is notable that the Laplace trans-

form transfer function of the circuit in Fig. 22.11 can be 

found by simply multiplying the Laplace transform of 



each stage, 


  
L[Vout (t)]
  

sτ1
H(s) = = . (22.108) 
L[Vin (t)] (1 + sτ1 )(1 + sτ2 ) 



The proof that the inverse transform of Eq. (22.108) 

yields Eq. (22.106) is left as an exercise. 


Example results for the shaping network of Fig. 22.11
are shown in Fig. 22.12, from which a few trends can be 
          
seen. First, as τ1 increases, more time is available to

measure the induced charge coming from the detector;        
hence, the total pulse height increases. Second, as τ2 Figure 22.12. Responses of a CR-RC network to a step
increases, the pulse height decreases. Third, as τ2 de- input voltage. The responses are labeled as τ1 , τ2 according
creases, the pulse height increases and also returns to to Eqs. (22.106) and (22.107).
1178 Nuclear Electronics Chap. 22

the baseline faster, thereby producing a faster pulse. To limit problems with pulse pile-up and dead time,
these time constants are usually kept short, on the order of a few microseconds.
However, if these time constants are made so short that they are comparable to the rise time of the
input signal from the preamplifier, similar to the charge collection time of the detector, then the input to the
CR-RC network no longer resembles a step function. Instead it appears as an impulse input with a much
different output than that depicted in Fig. 22.7(c). For instance, a square pulse input produces a truncated
exponential output that turns negative at the end of the pulse. This unfortunate outcome produces a lower
output pulse as a consequence of ballistic deficit. Hence, these time constants are generally designed to be
longer than the detector charge collection time. If, however, the time constants are too long, then problems
with electronic noise and pulse pile-up arise. As it turns out, for best performance, it is best to optimize the
operating system time constants according to the detector type and the radiation measurement environment.

22.2.9 (CR)2 -RC Network


Adding a second differentiator to a CR-RC network, or a
double RC differentiator, forms a bipolar output pulse of
V(t) C1 R2 C3
A=1
the shape depicted in Fig. 22.13. The Laplace transform
A=1 A=1
transfer function of this circuit is,
R1 C2 R3
s2 τ1 τ3
H(s) = . (22.109)
(1 + sτ1 )(1 + sτ2 )(1 + sτ3 )
For the fastest return to the baseline, a double differen-
time tiator circuit is usually designed with τ1 = τ2 = τ3 . The
advantage of the double differentiator is a reduction in
baseline undershoot compared to a unipolar response.
Figure 22.13. Depiction of a (CR)2 -RC circuit and the However, the bipolar pulse shaper usually has a reduced
resulting bi-polar output pulse. Here τ1 = R1 C1 , τ2 =
signal-to-noise ratio and a higher ballistic deficit than
R2 C2 , and τ3 = R3 C3 .
those of its unipolar counterpart [Nicholson 1974].

22.2.10 CR-(RC)n Network


2
A Gaussian output pulse should theoretically have a shape defined by e−(t/τ ) with a nearly optimum signal-
to-noise ratio from the symmetric shape. However, such an output is impractical, mainly because the pulse
shape would extend to infinity on both sides and, thus, have an infinite time response [Nicholson 1974].
Instead, a network can be devised to approximate a Gaussian output, typically one having several integrator
stages beyond the CR stage. The larger the number of integrator stages beyond the high-pass differentiator,
the closer the output is to an ideal Gaussian pulse. The Laplace transform transfer function is
sτd
H(s) = , (22.110)
(1 + sτd )(1 + sτ1 )(1 + sτ2 ) . . . (1 + sτn )
where τd is the differentiator (high-pass) time constant and n is the number of integrator (low-pass) stages.
If all integrator time constants are equal to τi , then
sτd
H(s) = . (22.111)
(1 + sτd )(1 + sτi )n
In practice, four integrator stages provide an adequately Gaussian pulse shape [Nicholson 1974]. The output
is defined by,  n
Vin t
Vout (t) = e−t/τ , (22.112)
n! τ
Sec. 22.2. Pulse Shaping 1179






 

   


  

  




      

       

Figure 22.14. Responses of a CR-(RC)n network to a step input voltage.


The responses are labeled as τ, n according to Eq. (22.112).

where n is the number of integrators beyond the low-pass filter. The additional shaping networks prolong
the pulse formation by the number n, and for equal values of τ the CR-(RC)n network is n times longer
than a CR-RC network. For instance, given equal values of τ , the CR-(RC)4 network has a pulse duration
4 times that of a CR-RC network. Also, because the shape is not a true Gaussian, the output pulse still
has slowly decaying tail. Consequently, pulse pile-up becomes more of an issue than with a CR-RC network.
However, if the time constants are adjusted such that the peaking time matches that of an equivalent CR-RC
network, the symmetry of the semi-Gaussian pulse enables it to return to the baseline more quickly and,
thereby to reduce pulse pile-up at high count rates. Example pulses calculated with Eq. (22.112) are shown
in Fig. 22.14. Notably, a practical Gaussian filter design usually incorporates active components (diodes,
transistors, op amps) rather than RC filters to produce the desired result [Ortec 2009a].

22.2.11 Delay Line Pulse Shaping


Another method of shaping a voltage pulse is to use two separate signal propagation paths for the input
signal. The outputs from each path arrive at different times and, when summed, change the signal. One
method used to accomplish this task is depicted in Fig. 22.15. At time t0 , the signal is split between two
paths. In the first path, the original signal propagates along the signal cable, such as a coaxial cable, and
arrives at the input of an amplifier at some time t1 . Also at time t0 , the signal is diverted through a
inverting amplifier with gain of unity,8 and then propagates along another cable, arriving at the input of the
second amplifier at time t2 slightly delayed behind the other signal. Hence, at time t2 , the second signal is
essentially subtracted from the first signal with delay Δt = t2 − t1√
. The pulse speeds v and arrival times are
determined by the cable characteristic properties, where v = 1/ LC (see Sec. 22.6 later in this chapter).
The signal delay can be determined by the difference in propagation times of the two transmission line cables.

8 Thisgain is at times referred to as a gain of −1. Throughout this text, the gain is the magnitude of the output signal to the
input signal, although the sign (negative or positive) of the output may change with respect to the input. Hence, the gain
here is 1, while the sign of the output is reversed with respect to the input.
1180 Nuclear Electronics Chap. 22

Dt
2R0 sum
1
vin vout
R0 LC R0
-1
(a) delay
invert

2R0 2R0
1 1
vin vout
R0 LC R0 R0 LC R0
-1 -1

(b)
Figure 22.15. Depicted are (a) a single delay line and a (b) double delay line for
shaping an input pulse. After Nicholson [1974].

Also, delay line amplifiers are available commercially as nuclear instrument modules (NIM) with a variety
of settings and delays. These instruments allow the operator to provide a signal to the module and change
the output by simply selecting different delay times and attenuations. The advantage of delay line shaping
is the rapid recovery or return to the baseline which cannot be realized with normal Gaussian shaping.
Suppose a step function is applied to the circuit of Fig. 22.15(a) at t0 = 0. One of the signals propagates
unaltered, except for attenuation from the cable resistance R0 . The other signal is inverted, attenuated also
by 2R0 , and delayed. When the inverted signal arrives at the summing junction at t2 , with delay of Δt,
it is added to the first signal. Because the delayed signal is negative, it causes the step pulse to become a
rectangular pulse of width Δt, thereby returning the output pulse to the baseline.
In practice, there is usually some additional attenuation in the delay line, and the added negative signal
may not completely restore the output pulse back to the baseline. This effect is especially pronounced for
exponential input signals. However, by making the value of 2R0 in the first cable adjustable, the signals can
be matched to eliminate this problem and properly return the shaped signal back to the baseline.
A bipolar shape can be formed by adding another delay line after the first, as depicted in Fig. 22.15(b).
Basically, it adds an inverted shaped pulse directly behind the original shaped pulse. With proper tuning of
2R0 , this method can also be used for exponential input signals. A disadvantage of the double delay line is
that the overall output pulse width is increased.

22.2.12 Pole-Zero Cancellation


The effects of poles and zeros in the transfer function of a circuit can cause the appearance of non-ideal
pulse shapes. For instance, the input to a common CR-RC filter usually has an associated input capacitance
Ci . The impedance across this capacitance is often regarded as infinite but usually is just very large.
Consequently, the input to the filter becomes
Q −t/τi
vin (t) = e (22.113)
Ci
rather than the desired step input.
Sec. 22.2. Pulse Shaping 1181

The equivalent circuit is shown in Fig. 22.16, which Rv


has the transfer function R2
sτi τ1 A=1 A=1 A=1
H(s) = . (22.114) C1
Ci (1 + sτi )(1 + sτ1 )(1 + sτ2 )
Ci Ri R1 C2
Consequently, this additional time constant τi = Ri Ci
produces an undershoot in the output pulse. Figure 22.16. Equivalent circuit for a CR-RC filter with
At least one method used to counter the effect is input capacitance Ci and pole zero compensation.
to place a variable resistor Rv across the C1 R1 stage
capacitance C1 [Nowlin and Blankenship 1965]. The new transfer function becomes,
τi 1 1
H(s) = +s . (22.115)
Ci (1 + sτi )(1 + sτ2 ) Rv + R1 Rv C1
+s
C1 Rv R1
Equation (22.115) is simplified with the substitutions
C1 Rv R1
τa = and τb = Rv C1 , (22.116)
Rv + R1
in which τb > τa , so that
τi 1 1
H(s) = +s . (22.117)
Ci (1 + sτi )(1 + sτ2 ) 1 τb
+s
τa
By adjusting the values of Rv , R1 , and C1 such that τa = τ1 and τb = τi , Eq. (22.117) reduces to
τ1
H(s) = , (22.118)
Ci (1 + sτ1 )(1 + sτ2 )
thereby eliminating the undershooting tail. It is common that linear amplifiers come equipped with a pole-
zero potentiometer in order to reduce or eliminate undershoot (or overshoot) of the shaped pulse. Note that
this compensated result is also achieved with Ri = Rv = ∞. Other pole-zero compensation methods for
more complicated input pulses are discussed by Blankenship and Nowlin [1966] and Strauss et al. [1967].

22.2.13 Base-Line Shift and Restoration


Amplifiers with AC coupled inputs often produce an output pulse with negative undershoot so the output
pulses are not unipolar, but rather have a bipolar characteristic. This effect is described earlier in Sec. 22.2.6
for a series of rectangular wave inputs to a passive high-pass filter. An example of the problem is depicted
in Fig. 22.8(b) and (d), in which the RC time constant τ is long compared to the cycle duration T .
The consequence of this undershoot problem is a shift in the base-line of the output pulse. Because the
output pulse is measured with respect to the actual zero, the measured amplitude is reduced from its actual
value. The problem is worsened in a real counting system because the input pulses arrive at random intervals
with random amplitudes. Although a simple counting system can suffer such a difficulty without significant
problems, a spectroscopy system suffers reduced energy resolution from the added deviation in pulse heights.
The base-line shifting problem increases with count rate, in which T is no longer much greater than τ .
Methods to counteract the base-line shift are described in the literature, including bipolar output, diode
clamping, and gated restoration [Nicholson 1974]. The bipolar method uses a circuit fashioned, in general,
after the concept shown in Fig. 22.13. Bipolar shapers have positive and negative lobes, and, hence, counter-
act the problem associated with base-line shifts. If the positive and negative lobes are of equal value, then
1182 Nuclear Electronics Chap. 22

the average value is zero and the output baseline remains unaltered. The consequence of bipolar shaping is
increased electronic noise and a high ballistic deficit. Many modern pulse shape amplifiers have monopo-
lar and bipolar shaping options, allowing the user to optimize the performance of the system by choosing
monopolar shaping for low count rates and bipolar shaping for high count rates.
The use of a diode in parallel with the resistor, shown
in Fig. 22.17(a), acts as a base-line restoration circuit. If
C C R at the time the base-line goes negative, t1 in Fig. 22.8(b),
vin R vout vin vout the diode is connected into the circuit and current flows
to ground. This flow causes the capacitor to charge up
opposite of the held charge and forces the output to re-
turn to zero. In reality, the diode has a small forward
(a) (b) resistance as does the signal source, both of which com-
bine to produce a small resistance Rs so that complete
Figure 22.17. Simple base-line restoration circuits with
(a) a diode clamp and (b) a gated switch.
restoration does not occur. The small negative pulse dis-
charges with time constant RC, and recharge with the
next pulse by time constant Rs C. However, if the time constant RC is much greater than T , then the
base-line is essentially clamped to zero. In reality, the single diode design is capable of restoring base-line
shifts in only one direction. Robinson [1961] and Fairstein [1975] solve this problem by placing two diodes
in the circuit to adjust base-line shifts in either direction. Various base-line restoration designs with diode
clamps are discussed by Nicholson [1974].
Another method used to restore the base-line is with a gated switch, depicted in Fig. 22.17(b). This
configuration eliminates the base-line shift from changing count rates. The switch is open during the input
pulse and closed when the output pulse turns negative. By doing so, the CR circuit is active only between
pulses, when the voltage is restored to zero. The switch is usually a combination of diodes [Robinson 1961],
or more complex circuitry (see references in Nicholson [1974], Karlovac and Blalock [1975] and Fairstein
[1975]). The stability of base-line restoration at high counting rates depends on the ability of the gating
control circuits to distinguish between the incoming pulses and the base-line. This discrimination can be
achieved with a manually adjusted discriminator set slightly above the electronic noise straddling the base-
line. Such sophisticated amplifiers include automatic noise discriminators and complicated pulse detection
techniques that effectively perform this task [Karlovac and Blalock 1975; Fairstein 1975].

22.3 Components
The main electronic components commonly used in a radiation detection system were introduced in Chapter
2, primarily because many readers using this book to learn about radiation detectors might also need to use
some of these components in a laboratory setting as they gain knowledge about the operation of radiation
detectors. In the following sections, additional information about these components is provided.

22.3.1 Preamplifiers
A preamplifier unit has two basic purposes, namely (1) to provide a low-noise coupling of the typically
high impedance of the detector to a low impedance capable of driving the string of amplifier and readout
electronics, and (2) to produce a first stage of signal amplification. This first stage of amplification is
usually small. Preamplifiers are designed to be either voltage sensitive, current sensitive, or charge sensitive.
Optimum detector performance is obtained when the type of preamplifier is properly matched to the type
and characteristics of the detector and the analysis electronics.
Sec. 22.3. Components 1183

Voltage-Sensitive Preamplifiers
Consider the simple preamplifier shown in Fig. 22.18. A resistor
R1 is connected between the input voltage and terminal 1 while i2
summing
terminal 2 is grounded. Also, a feedback resistor R2 is connected junction
between terminal 1 and terminal 3. The current flowing through R2
R1 is described by, i1
vin − vA vA 1
i1 = (22.119) +
R1 R1
+ vAB A
and the current flowing through R2 is vin 3
+
vA − vout vB 2
+ vout
i2 = . (22.120)
R2
The small voltage appearing between terminals 1 and 2 is,
Figure 22.18. Simple voltage sensitive pream-
vAB = vB − vA , (22.121) plifier with the inverted configuration.

but because terminal 2 is grounded VB = 0 so that

vAB = −vA . (22.122)

Because the input impedance into the op amp is large, only an insignificant current flows into terminal
1. Hence, the current flowing through R1 also flows through R2 , i.e., i1 = i2 , so equating Eqs. (22.119) and
(22.120) gives
vin − vA vA − vout
= , (22.123)
R1 R2
or, upon rearrangement,
vout R1 − vA (R1 + R2 ) = −vin R2 . (22.124)
Equation (22.36) for the present analysis becomes
vout
= vB − vA = −vA (22.125)
A
because here vB = 0. By combining these last two equations, the transfer function of this preamplifier is
vout AR2
=− . (22.126)
vin [R1 (A + 1) + R2 ]
This result can be significantly simplified by recognizing that the open loop gain A is very much larger than
unity so that R1 (A + 1) R2 and, consequently, Eq. (22.126) reduces to,
vout R2
− . (22.127)
vin R1
This simple result can also be obtained as follows. Conceptually, one can think of terminal 1 being at
virtual ground and causing the input voltage at terminal 1 to also be zero. This means that the current
flowing through R1 must be equal to i1 = vin /R1 . However, the input impedance of the op amp prevents
current flow into the device. Instead, the current i1 must flow through R2 , thereby producing a voltage
equivalent to vin R2 /R1 . At terminal 3, the output voltage vout is
R2
vout = v1 − i1 R2 = 0 − vin , (22.128)
R1
1184 Nuclear Electronics Chap. 22

which yields the same transfer function as Eq. (22.127).


The gain of Eq. (22.127) is called the closed loop gain. First, note that ideally the open loop gain A has
no bearing on the closed loop gain.9 Second, the gain produced has the opposite or inverse sign of the input,
hence the name for this circuit is the inverting configuration. The inverting configuration is a common circuit
used as a voltage sensitive preamplifier, so named because they tend to respond to and linearly amplify the
voltage input from the detector into the preamplifier circuit.
As discussed in Chapter 8, the voltage input vin into the preamplifier from the detector is generally an
inverse function of the detector capacitance, vin ≈ Qi /Cd , where Qi is the charge induced by the motion of
electrons and ions excited in the detector by a radiation interaction event and Cd is the combined capacitance
of the detector and coupling cables. Hence, to reduce the capacitance, the preamplifier circuit is usually
placed as close as possible to the detector without causing environmental damage to the circuit.
For many detectors, the capacitance remains constant for different applied operating voltages Vo ; hence
the preamplifier output vout is mostly linear with respect to the charge excited in the detector regardless of
the voltage applied to the detector. Examples include gas-filled detectors and scintillation detectors that are
coupled to photo-multiplier tubes.
Now consider the circuit of Fig. 22.19, referred to as the
non-inverting preamplifier configuration. It looks similar to the
inverting configuration, except that the voltage input is now at
vin
vB 2 + the positive terminal, denoted with the present convention as
+ + 3 input 2. As before, the output at terminal 3 is
vAB A
+ vout = A(vB − vA ). (22.129)
vA 1 vout
The voltage at input 2 is vB = vin so that Eq. (22.129) gives
i1
i2
vout + AvA
R1 = vin . (22.130)
R2 A
From Fig. 22.19 it is seen that
Figure 22.19. Preamplifier in the non-inverting  
configuration.
R1
vA = vout . (22.131)
R1 + R2

Substitution of Eq. (22.131) into Eq. (22.130) and rearrangement of terms yields

vout A(R1 + R2 )
Gain = = . (22.132)
vin (A + 1)R1 + R2

Notice that the output voltage vout retains the same polarity as the input voltage vin . The gain of Eq. (22.132)
is often simplified with the assumption that A is very large, so that Eq. (22.132) reduces to

vout R1 + R2 R2
Gain = ≈ = + 1. (22.133)
vin R1 R1

However, if the A + 1 is not much larger than the ratio (R2 + R1 )/R1 , then considerable error can occur if
the approximation of Eq. (22.133) is used.

9 Inreality, the rolloff of the open loop gain has a significant effect on the signal gain of the amplifier. See Carter and Brown
[2016], Carter and Mancini [2017], Jung [2005], and Zumbahlen [2008] for more details.
Sec. 22.3. Components 1185

Current-Sensitive Preamplifiers
A current-sensitive preamplifier is designed to measure the instantaneous current flowing from a detector.
The practical implementation of the topologies can be identical for charge sensitive and current-sensitive
preamplifiers, but they are used for different purposes. The component values are optimized to extract
different information. This current sensitive preamplifier is seldom used for most detector applications;
however, on rare occasion a preamplifier with a fast rise time for timing applications is needed, and a current
sensitive preamplifier is required. Examples in which a current sensitive preamplifier is needed include timing
applications with fast photomultipliers and microchannel plates. The current sensitive configuration requires
that the input impedance be low and the preamplifier gain A be very large. These conditions can be realized
by using the general design of a voltage sensitive preamplifier and reducing the load resistance at the input
of the preamplifier.
A simplified current sensitive preamplifier is depicted in i2
summing
Fig. 22.20.10 The two resistors form a parallel circuit so that junction
the current flowing in R1 is R2

R2
iin vA 1
i1 = iin . (22.134) +
R2 + R1
+ vAB A 3
If R1 is much smaller than R2 , then Eq. (22.134) indicates vin i1 R1 +
that i1  iin so that vout  −AvA = −Ai1 R1 . If the in- vB 2
+v out
put impedance is 50 Ω, then it can be impedance matched
to a common 50 Ω transmission line, thereby eliminating re-
flection losses. The current sensitive preamplifier converts Figure 22.20. Simple current sensitive pream-
the input current iin to an output voltage vout described by plifier with the inverted configuration.
vout  Aiin (50Ω).
Because current sensitive preamplifiers are designed to track the detector signal for timing purposes,
noise added to the signal causes uncertainty in the actual arrival time of a pulse. This uncertainty is called
jitter. A preamplifier rise time that is faster than the detector signal really does not help the situation.
First, the output signal cannot be faster than the input signal, so a preamplifier rise time that is much faster
than the input signal offers no real advantage. Instead, more noise is accepted into the system, thereby
causing more jitter. By contrast, if the preamplifier signal is much slower than the detector signal, then the
timing resolution suffers. To minimize the effect of jitter, Cova et al. [1991] recommend that the preamplifier
rise time be similar to that of the detector input. For practical applications, it is recommended that the
preamplifier rise time be within a factor 2 of the detector rise time [Ortec 2009b]. Note that the Johnson
noise can be high unless the feedback resistor in the preamplifier circuit is R2 ≥ 109 Ω [Nicholson 1974].
Charge-Sensitive Preamplifiers
There are some detectors that change capacitance as voltage is applied, particularly semiconductor diode
detectors. These semiconductor detectors have depletion regions (Chapter 15) that increase with applied
operating voltage, which, in turn, causes the capacitance Cd to decrease with increasing voltage. As a
result, the preamplifier output changes with a varying operating voltage for identical induced charges qi . By
redesigning the preamplifier feedback circuit, the capacitive component of the detector Cd can be minimized
compared to the feedback capacitance Cf of the preamplifier, thereby effectively rendering the preamplifier
output almost entirely dependent upon the induced charge qi .
Consider the amplifier circuit shown in Fig. 22.21. There is a capacitor C1 connected to input terminal 1
and another capacitor C2 connected across terminals 1 and 3. The capacitor C2 is referred to as the feedback

10 Insome cases, the feedback resistor R2 is missing from an idealized current sensitive preamplifier diagram, implying that it
has an infinite feedback resistance.
1186 Nuclear Electronics Chap. 22

capacitor, often denoted Cf . The voltage vin stored on C1


v2 appears at the summing junction. The voltage at the summing
summing
junction junction is vin and must equal the voltage across C2 plus vout ,
C2
i.e.,
vA 1 vin = vout + v2 . (22.135)
+
+ A For an ideal op amp vout = −Avin so that Eq. (22.135) can be
vAB 3
vin v1 C1 + written as
vB 2
+ vout (A + 1)
v2 = (A + 1)vin = − vout . (22.136)
A
Figure 22.21. Simple charge sensitive pream- Because v2 = q2 /C2
plifier with the inverted configuration.
q2 (A + 1)
=− vout , (22.137)
C2 A
which upon rearrangement gives
A q2
vout = − . (22.138)
(A + 1) C2
Because A is very large and q2 is the induced charge qin from the detector
qin
vout  − . (22.139)
C2
The important outcome of Eq. (22.139) is that the output voltage is a function of the feedback capacitor
C2 and the induced change qi and does not depend on the detector capacitance. Hence, for semiconductor
diode detectors, the voltage output vout is largely dependent only upon the induced charge qi and feedback
capacitance C2 , where vout = −Avin ≈ −qi /C2 , where A is the preamplifier gain. The charge gain is then
vout 1
=− . (22.140)
qin C2
The goal of the detector system is to measure all of the charge generated in the detector. However, some
charge remains on the sensor capacitance, leading to the following ratio for the input charge to the amplifier
to the charge remaining on the detector [Spieler 2005],
qin vin Cin 1
= = . (22.141)
qin + qdet vin (Cin + Cdet ) Cdet
1+
Cin
where Cin is the dynamic input capacitance of the preamplifier. For Cin Cdet , the ratio Qin /(Qin + Qdet )
approaches 100%.
Commercial charge-sensitive preamplifiers are designed for optimum performance when matched to spe-
cific ranges of detector capacitance. Hence, it is advised that the user consult the preamplifier specification
sheets to properly match detectors to preamplifiers.

Example 22.5: Consider a silicon surface barrier detector connected to a commercial preamplifier with
input capacitance of 10 nF. The detector is circular with diameter of 15 mm. The background doping
concentration is 1013 cm−3 with Vbi = 0.3 volts. What is the charge ratio measured at self-bias volts? What
is it at reverse bias of 150 volts?
Sec. 22.3. Components 1187

Solution:
From Chapter 15, one uses the depletion approximation for the detector self-bias capacitance,
−1/2 1/2
κ0 A 2κ0 (Vbi − V ) qNb κ0
Cdet = = κ0 πr 2 = πr 2
L qNb 2(Vbi − V )

1/2
π (1.6 × 10−19 C)(1013 cm−3 )(11.9)(8.854 × 10−14 F cm−1
= (1.5 cm)2
4 2(0.3 V)

= 2.962 nF.

Recalling that the depletion width increases with V , the capacitance at 150 volts reverse bias is,
 
Vbi 0.3
Cdet = 2.962 pF = 2.962 pF = 132.34 pF.
V + Vbi 150.3

For the self-biased case,

Qin 1 1
= = = 0.7715 or 77.15%.
Qin + Qdet Cdet 2.962 nF
1+ 1+
Cin 10 nF
By the way, the resulting depletion layer width is only 6.29 microns, relatively small compared to alpha
particle ranges from most check sources, meaning that the depletion region would be too small to absorb the
total particle energy. Consequently, the charge that is deposited in the depletion capacitance is less than
the total amount liberated, further diminishing the measured charge.
For the case where the detector is reverse biased at 150 volts,

Qin 1 1
= = = 0.9869 or 98.69%.
Qin + Qdet Cdet 132.34 pF
1+ 1+
Cin 10 nF
Also, the depletion depth would be 140.7 microns, wide enough to absorb alpha particle energies up to
approximately 15 MeV.

Charge Sensitive Preamplifier with Resistive Feedback


The charge stored across the feedback capacitor in the charge-sensitive configuration shown in Fig. 22.21
accumulates with successive inputs, and eventually the charge reaches the limiting storage capacity. In
order to discharge the capacitor between input pulses, a resistor is attached in parallel across the feedback
capacitor so the capacitor discharges exponentially with a decay time constant of τ = RC.11 These time
constants can be relatively long and are often about 50 μs [Ortec 2009a].
Pulse pile-up, depicted in Fig. 22.1, is due to subsequent pulses arriving before a prior pulse has returned
to the base-line. Although the circuit ideally does not suffer from dead time losses, the output pulses are
distorted. If the pulse decay tail is positive, then the subsequent pulse magnitude is greater than it should
be, as shown in Fig. 22.1(a). If the pulse decay tail suffers undershoot, then the subsequent pulse is less than
it should be, as shown in Fig. 22.1(b). In either case, the result is a broadening of the pulse height spectrum
which reduces the energy resolution of the spectrometer. Further, at high count rates, multiple pulses

11 Note that the value selected for this resistor is critical to stability of the preamplifier.
1188 Nuclear Electronics Chap. 22

contribute to the pile-up problem and the total magnitude of the stored charge can exceed the preamplifier
limit to produce a condition called “saturation overload,” as shown in Fig. 22.22.
Because preamplifier output pulses are usually sent to the input of a shaping amplifier, the amplifier
output can be affected by these pulse height distortions created by the preamplifier. There are several
amplifiers designed to address pulse pile-up distortions, a few of which are described in latter sections.

Pulsed-Reset Preamplifiers
The pulsed-reset preamplifier was designed to reduce noise contribu-
V(t) tions from the feedback resistor by eliminating it altogether. In other
overload level words, R can be regarded as being infinite. Consequently, the decay
constant of the feedback capacitor is essentially infinite so the decay
tail now becomes a flat step (see Fig. 22.23(a)). Each input to the
preamplifier produces a step increase in voltage proportional to the in-
put charge of each pulse. During charge integration, the system does
not suffer from dead time, mainly because the preamplifier continues
to integrate the input charges that produce the stair-step output. The
time step inputs are shaped by a shaping amplifier, as described in previous
Figure 22.22. Preamplifier pulse sections. However, if two input pulses occur too close together, a form
pile-up output at high counting rates. of pile-up occurs at the shaping amplifier which can cause pulse-height
Pulses can become distorted if they ex- distortions.
ceed the preamplifier overload level.
A consequence of this preamplifier design is that the feedback ca-
pacitance does not discharge the accumulated charge as would occur in a resistive feedback preamplifier. To
remedy this problem, an active reset method is incorporated. When the charge accumulated on the feed-
back resistor reaches a predetermined voltage, labeled Vramp , a reset sequence begins. The design generally
replaces a resistor in the feedback loop with either a light emitting diode (LED) or a transistor [Landis et
al. 1971; Landis et al. 1982], either one being activated at the end of T2 to reset the feedback capacitor.
First, a short time duration is allowed that passes the last valid input pulse, labeled T2 in Fig. 22.23(a).
The capacitor is rapidly discharged during T3 using an optical or transistor feedback method. In the case
of optical feedback, a light-emitting diode (LED) is triggered that illuminates an optical gate such as a
field effect transistor (FET), which opens and discharges the feedback capacitor. Optical feedback has been
largely replaced by active FET discharging, in which the gate on the FET is opened to discharge the feedback
capacitor when the reset voltage is exceeded.
In either case, the rapid discharge can produce a negative output from the shaping preamplifier. To
prevent a negative output, the preamplifier remains disabled for a preset time, designated Taol . During
this disabled period, a blocking signal can be supplied to the shaping amplifier for a time Tinh to prevent
the output of erroneous signals. Although the fractional dead time of the preamplifier would ideally be
expressed by the ratio of T3 /T1 [Britton et al. 1984], the actual fractional deadtime is determined by the
time the amplifier cannot accept pulses. Hence, the fractional system deadtime is represented by

Tinh Tinh
DTf = = , (22.142)
T1 Vramp
+ T2 + T3
(ER)(CG)

where ER is the input rate of energy into the preamplifier and CG is the conversion gain of the energy to
voltage pulse height.
Sec. 22.3. Components 1189

T3 T3
T2 T2
Reset Voltage
amplitude

(a) Vramp

T1
Taol
(b)

Tinh

(c)
time

Figure 22.23. Output waveforms from a pulsed-reset preamplifier, where (a)


is the output from the preamplifier, (b) are shaped pulses from a Gaussian
amplifier, and (c) is the inhibit signal activated to stop data collection during
the reset time. After Britton et al. [1984].

22.3.2 Amplifiers
The output pulse from a preamplifier is usually designed to have a short rise time τrise and a long fall time
τf all so that τrise  τf all . Often another radiation interaction occurring in the detector arrives before the tail
pulse from the previous radiation interaction is completely discharged. Consequently, subsequent pulses ride
atop the tail of prior pulses, as shown in Fig. 22.22. The size of the step increase from a tail pulse contains
information about the energy deposited in the detector because it is proportional to charge produced by
an interaction and subsequently measured by the preamplifier. Hence, one purpose of the amplifier chain is
to measure that signal increment and shape the resulting measured signal into a much shorter pulse signal.
Also, because the gain of a preamplifier is usually small in order to prevent overload, the step change is
difficult to measure accurately and the small signal can be attenuated significantly over relatively short cable
distances. The purpose of the amplifier is to address both of these issues. First, to shape the charge by
producing a significantly faster output pulse that still preserves the differential step change of each pulse.
Second, to provide additional amplification of the signal. In some cases, fast timing amplifiers allow the
preservation of information about the arrival time of different input pulses.

Linear Amplifier
For spectroscopy systems, the preferred amplifier choice is a linear pulse shaping amplifier. The amplifier
serves to shape and amplify the input pulses from the preamplifier and produces an output whose amplitude
is usually restricted by the maximum 10-volt NIM standard. Thus amplification of a pulse over the maximum
limit results in a clipped output with the shaped pulse output being truncated at 10 volts in case of the NIM
standard. Users are well advised to adjust the gain such that output pulses for the radiation energy under
inspection is well below 10 volts.
1190 Nuclear Electronics Chap. 22

oscilloscope

discriminator
detector preamplifier amplifier or SCA counter/timer

040657
g-ray
1

MCA

+ - 2
power supply

Figure 22.24. Detection system and components for either pulse counting (with SCA) or
energy spectroscopy (with MCA).

Most linear amplifiers allow the user to ad-


 just the shaping times, with research units hav-
 
  % 
 
  %  ing adjustable independent rise and fall times.
 
  % 
 
  % 
This feature allows the user to optimize the

&   '  %  energy resolution performance of the system.
&   '  % 
Gaussian shaping is common with linear shap-
!"#$


ing amplifiers, although some units offer differ-
 ent shaping outputs such as triangular or qua-
sitriangular as well as variations of Gaussian
 shaping. Shown in Fig. 22.25 are data obtained
for different shaping networks at different count
rates for an HPGe detector. As can be seen, the
energy resolution changes with shaping time.

           The minimum FWHM also changes as the count
      rate changes. From results such as those shown
in Fig. 22.25, the shaping times of a linear pulse
Figure 22.25. The energy resolution as a function of the pulse amplifier can be adjusted to give the best energy
width for linear amplifiers with three different shaping networks. resolution. If the shaping times selected are too
Also shown are the results from two different counting rates (2000
cps and 62000 cps). Data are from Fairstein [1985].
short, then ballistic deficit losses worsen the en-
ergy resolution and the FWHM widens. Also,
the contribution from series noise (see Sec. 22.7) increases and consequently decreases the energy resolution.
If the shaping time is too long, then parallel noise contributions increase, which also compromises the energy
resolution. As the count rate increases, the effects of pulse pile-up also begin to affect detrimentally the
energy resolution if long shaping times are used. Consequently, the shaping time should be adjusted for
optimum performance at the pulse rate under inspection.
For high-resolution HPGe detectors, the shape of the detector pulse varies depending on the location
of the radiation interaction. The induced current entering the preamplifier changes as a function of the
Sec. 22.3. Components 1191

weighting field in the detector, which is a function of position in the detector, so that the rise time of the
pulse is also a function of the interaction location (see Sec. 16.4). As a consequence, less charge is integrated
per unit time for long rise times, while the opposite is true for short rise times. If the shaping time is
adequately long, then this effect is minimal because most of the charge is integrated regardless of the rise
time. However, if the shaping time is short relative to the rise times, then there is detrimental increase in
the variance of the output pulses from the preamplifier for monoenergetic events. This problem is called the
ballistic deficit (see Sec. 22.2).12 For low count rates, the shaping time can be set relatively long (> 6 μs)
to reduce the effects of ballistic deficit. At high count rates, short shaping times are preferred in order to
reduce pulse pile-up. However, shaping times shorter than 2 μs can cause energy resolution to degrade in
high-resolution HPGe detectors [Becker et al. 1981]. Commercially available spectroscopic linear amplifiers
quote the spectral broadening for high radiation interaction rates in the detector.13

Gated Integrator
Karlovac and Blalock [1975] describe a method for preserving the energy resolution despite a ballistic deficit
caused by short shaping times needed for high interaction rates in the detector. The method uses a time-
variant amplifier, or “gated integrator,” to process the pulse [Radeka 1972]. An output pulse from a semicon-
ductor detector, typically an HPGe detector, is introduced through a preamplifier into a Gaussian shaper.
This Gaussian shaper with a short time constant rapidly shapes the input from the preamplifier and delivers
the shaped pulse to the gated integrator. The charge leaving the Gaussian shaper is stored on a feedback
capacitor across the gated integrator. This charge is the integral (area) of the pulse. At a preset collection
time, a shorting gate closes across the feedback capacitor to fully discharge it to ground, while another gate
is opened to disconnect the Gaussian shaper from the gated integrator during the discharge process. The
time that the gated integrator is active is much longer than the Gaussian shaping time, usually on the order
of 10 microseconds. The Gaussian shaper must remain active long enough to measure all charge from the
detector.
This gating technique is demonstrated in the modeled results of Fig. 22.26. Here the inputs of three
identical charge packets are applied to a fast Gaussian shaper with 0.7 μs shaping time. In one case, the
induced current is high from fast charge collection (10 ns) and the Gaussian shaper develops the full Gaussian
output with no ballistic deficit. In a slightly slower case, the shaping time and the charge collection time
(1 μs) are comparable. Hence, a small amount of ballistic deficit is observed, but the overall integrated output
reaches the same level as the faster pulse. In the third case, the charge collection time (10 μs) is much slower
than the shaping time. After a short rise, the output fall time causes the input signal to match the output
signal, forming a flat top pulse. However, the integral of this slower pulse also reaches the same output as
the faster pulses, albeit at a much later time. The integrated charge, shown for all inputs, eventually reaches
the same value, despite the rise time differences. The total charge is the same in all cases and is stored on
the gated integrator capacitance. Consequently, the output is no longer based on the pulse height as with
time-invariant linear amplifiers, but instead the total integrated charge in the pulse. The output is therefore
independent of the ballistic deficit perturbations and no longer affects the gated integrator output pulse
magnitude, provided that all charge is collected during the processing time and there is no pulse pile-up

12 Note that ballistic deficit is a consequence of using too short of a shaping time, which results in lost charge integration. For
short shaping times, the ballistic deficit can also be affected by specific current induction, which varies as a function of the
interaction location, carrier velocity, and the weighting field in the detector [Radeka 1972].
13 The spectral broadening in terms of percent at a specific high “count rate” is used for this metric. However, this description

is somewhat imprecise, because the count rate is the observed response from a system; whereas, it is the input pulse rate that
causes the problem. A high input pulse rate is produced by a high radiation interaction rate in the detector and this leads to
pulse pile-up. The ballistic deficit is thus exacerbated by short pulse shaping times.
1192 Nuclear Electronics Chap. 22

Figure 22.26. Modeled pulses from a Gaussian shaper with τ = 0.7μs, showing the
effects of different carrier drift times for the same amount of total charge. Also shown is
the integrated output, with gain of 500,000, obtained from the shaped signals. In (a), the
drift time is 10 ns, yielding a semi-Gaussian output with negligible ballistic deficit. In
(b) the drift time is 1 μs and in (c) the drift time is 10 μs. Although the Gaussian peak
voltage is different for all cases, the integral of the signals is the same for all cases. Hence,
provided that all charge is collected during the processing time and there is no signal
pile-up, the integral can be used to preserve the detector spectroscopic information.

during the signal shaping and integration process. Because the circuit is designed to operate under high
interaction rates, pile-up rejection is used to reject overlapping pulses.
Two advantages of the gated integrator amplifier circuit are apparent. First, the energy resolution
is preserved because ballistic deficit from different rise times is no longer a problem. Second, a shorter
time constant allows faster pulse processing; hence more counts are recorded at high rates of gamma-ray
interactions. Because the system dead time is largely determined by the processing times of the gated
integrator and that of the multichannel analog-to-digital processor, changes in the observed count rate do
not necessarily track the interaction rate in the detector [Simpson et al. 1991]. The example spectra in the
work of Karlovac and Blalock [1975] shows good energy resolution for an interaction rate of 150,000 gamma-
rays per second, but records only (approximately) twice as many counts as observed for a lower count rate
of only 5000 interactions per second.14
Details for the Common Linear Amplifier
Ideally, a linear pulse amplifier should have the following properties. The output of the amplifier should scale
proportionally to the energy input, a condition requiring that any integral and differential non-linearities

14 The literature states the that input is 150,000 counts per second (150 kcps) [Karlovac and Blalock 1975], but this is a semantics
problem. Strictly, the observed count rate is the final tally allowed by the system, which is seriously lower than the gamma-ray
interaction rate in the detector. The authors of this text believe that interaction rate, not count rate, is what Karlovac and
Blalock actually meant.
Sec. 22.3. Components 1193

should be small. For a linear preamplifier, the minimum output is 0 10 volt limit

voltage
output
volts, while the maximum output (NIM rules) is 10 volts. Hence, the
minimum input should result in 0 volts output, while the maximum vm
allowed input yields 10 volts output. Ideally the output voltage scales videal
linearly with the input voltage, as depicted in Fig. 22.27. However, vo2m
there usually is some non-linearity, i.e., ideal
vo2i
vout
= A (1 + int ) , (22.143) vo1m
vin
vo1i
or
vout − Avin
int = , (22.144) vi1 vi2 input
Avin voltage
where A is the gain and int is the integral non-linearity [Kowalski
Figure 22.27. Examples of integral
1970]. The differential non-linearity dif is defined as and differential non-linearity in an am-
plifier output.
dvout
= A (1 + dif ) , (22.145)
dvin
or
dvout 1
dif = − 1, (22.146)
dvin A
which describes non-linearity between small differences in pulse heights.
Both non-linearities can be measured from a plot of vout versus vin such as shown in Fig. 22.27. For any
given input vin the integral non-linearity of Eq. (22.144) is
vm − videal
int = (22.147)
videal
where vm is the measured output and videal is the predicted linear output.15 The differential non-linearity
can be determined from the ratio of slopes of the measured outputs to linearly predicted outputs at any
input voltage, i.e.,
   −1     −1 
vo2m − vo1m vo2i − vo1i vo2m − vo1m A (vi2 − vi1 )
dif = lim −1= lim −1
vi2 →vi1 vi2 − vi1 vi2 − vi1 vi2 →vi1 vi2 − vi1 vi2 − vi1

vo2m − vo1m
= lim − 1, (22.149)
vi2 →vi1 A(vi2 − vi1 )
where vo2m and vo1m are measured outputs and vo2i and vo1i are ideal outputs, both corresponding to inputs
vi2 and vi1 , respectively. Usually, these metrics are reported for the highest observed non-linear behavior over
the output voltage range. Commercial spectroscopy linear amplifiers usually have an integral non-linearity
≤ ±0.025% between 0 to 10 volts, and a differential non-linearity ≤ ±0.012% between -9 to 9 volts.
Another problem that can occur with linear amplifiers is in the amplification of small pulses in the presence
of large pulses. If sufficient gain is used to distinguish small pulses from large pulses, the processing of a

15 To provide a uniform measure over the amplifier range, integral non-linearity for commercial units is often reported as,
vm − videal
int = , (22.148)
vmax
where vmax is the 10 volt NIM limit. Usually it is the highest measured value of int over the amplifier range that is reported.
1194 Nuclear Electronics Chap. 22

large pulse may result in a clipped output in


V(t) which the pulse exceeds the overload setting. Con-
clipped
pulse sequently, the pulse undershoot, as shown in
Fig. 22.28, of this overload pulse is also large, and
small the recovery takes excessive time to return to the
pulse base-line. During the recovery time, small pulses
time that arrive are distorted by the negative tail of the
overloaded pulse. Modern systems have overload re-
undershoot sistant circuits that minimize this effect. Commer-
Figure 22.28. Overload pulses can have large undershoot and cial spectroscopy amplifiers usually have the over-
long recovery time. Small pulses arriving during the recovery load recovery specifications reported for maximum
time of an overload pulse are distorted. gain on the performance sheet.
Thermal stability is important, and the gain
should not drift with temperature changes. Commercial units usually have thermal stability of ≤ ±0.0075%
per ◦ C within a specified temperature range (typically between 0 to 50◦ C). Also electronic noise must be
relatively low to achieve high energy resolution. Hence, the signal-to-noise ratio must be optimized for
the device by adjusting the shaping times to coincide with the highest energy resolution (see, for example,
Fig. 22.25). The amplifier should respond to high pulse input rates with negligible pile-up effects. Finally,
there are some cases where the time correlation of the input pulse must be preserved, and the time trigger
method becomes important as explained in the next section.
Amplitude adjustment includes coarse increment changes from 5× up to a maximum gain (usually 2000×).
Most units also have a fine adjustment feature, with a continuously adjustable scaling factor between 0.5× to
1.5×. These features allow the user to adjust a pulser input to precise amplitudes for calibration purposes,
or to adjust the shaped detector input to fall within the desired range of pulse heights. Detection systems
and components for common counting and spectroscopy applications are shown in Fig. 22.24. Other features
common to a linear spectroscopy amplifier are pole zero adjustment, automatic base-line restoration, pulse
pile-up rejection, and choice of unipolar and bipolar outputs.

Timing Amplifier
For measurements where time correlation is important, the electronic pulse is sent to a timing pick-off gate
that uses a threshold method to trigger a time stamp on the pulse. If the pulse height coming from the
detector or preamplifier is too low to surmount this threshold, some amplification is then required that does
not alter the time signal of the pulse. Common linear amplifiers are not well suited for this purpose, but are
instead designed to eliminate high frequency noise while preserving the energy information provided by the
detector. Hence, a fast timing preamplifier is needed that mimics the input signal with the added benefit
of gain. Timing amplifiers may have rise times in the range of nanoseconds or smaller. Unfortunately, such
fast rise times can also detrimentally affect linearity, thermal stability, and electronic noise. Because such
amplifiers were designed to process negative output pulses from PMT anodes, the pulse polarity output of
commercial units is usually negative to remain compatible with fast timing discriminators.
Earlier it was shown that AC coupling could be used as a DC filter while passing higher frequency
signals. Hence, a wideband amplifier may be DC coupled to extend the frequency response to zero while still
responding to high frequencies. Wideband amplifiers offer no control over the rise time or the decay time
of the signal. Also, wideband amplifiers are best used with photomultiplier tube output signals and with
silicon diode detectors to preserve timing information [Ortec 2009a]. Pulse shaping adjustment controls are
provided with timing filter amplifiers, and they also typically have base-line restoration electronics. This
type of timing amplifier is generally useful for timing applications with high-resolution HPGe detectors. For
timing applications with either type of amplifier, the rise time should be selected to be less than the inherent
Sec. 22.3. Components 1195

clipped

pulse height

10 volt limit
10 volt limit

frequency
accepted

(a) LLD

rejected

time

LLD
pulse height

clipped
pulse height

10 volt limit
10 volt limit

rejected frequency

ULD

DE accepted
(b) LLD

rejected
E

pulse height
ULD

time
LLD

Figure 22.29. The function of an (a) integral discriminator and a (b) single channel analyzer.

rise time of the preamplifier to reduce or eliminate degradation of the signal rise time. As already noted
in the discussion on current-sensitive preamplifiers, the rise time should be faster than the input signal rise
time, yet not too much faster or electronic noise becomes a problem. Consequently, excessively fast amplifier
rise times should be avoided, because they introduce more noise and provide no additional improvement in
the signal rise time. The differentiator time constant should be set just large enough to avoid significant loss
of the signal amplitude.

22.3.3 Integral Discriminators and Single Channel Analyzers


The electronic pulses emerging from a shaping amplifier are indicative of the energy absorbed within the
detector. The amplitude of the pulse varies linearly with the absorbed energy in a well-designed system.
Hence, once calibrated, the final signal pulse height is a measure of the energy absorbed in the detector.
The main function of both discriminators and single channel analyzers is to reject shaped pulses outside
established pulse-amplitude boundaries, thereby passing only pulses whose amplitude voltages are of interest.
These systems convert a shaped input pulse into a logic output pulse, usually triggered when the leading
edge of the shaped pulse surpasses a preset voltage threshold. Because the output is a logic pulse, energy
information is preserved by the electronic boundaries set by the user and not the output pulse amplitude.
Logic pulses are characterized by a binary system, consisting of lows and highs, or alternatively as 0s and
1s. For instance, the Nuclear Instrument Module (NIM) system logic pulse is low (0) at 0 volts and high
1196 Nuclear Electronics Chap. 22

(1) for a current of -16 mA through a 50Ω resistor, or a voltage of -0.8 volts.16 The integral discriminator
allows the user to select a signal voltage or energy E defined by a lower level discriminator (LLD) threshold,
below which all pulses are rejected (depicted in Fig. 22.29(a)). In most models, any signal above the LLD
is passed. However, some systems reject pulses that exceed the nuclear instrument module standard 10-volt
upper limit. Because all pulses above the setting E are counted, 10 volt-limit notwithstanding, this device
essentially passes all signals above the threshold. Hence, the accumulated pulses during the counting time
is the integral of the pulses above E.
Unlike the integral discriminator, the single channel analyzer (SCA) is designed to filter out pulses whose
amplitudes are both below a lower level discriminator (LLD) and above an upper level discriminator (ULD)
setting. The LLD threshold is designated by E, a relative pulse height energy, while the ULD threshold is
designated E + ΔE where ΔE is the width of the energy channel. Hence, the SCA allows the user to pick a
voltage window (or energy window) of interest defined by lower and upper energy thresholds, and pass only
those signal pulses that fall within those boundaries, as depicted in Fig. 22.29(b).
One method to accomplish this filtering task is to set two adjustable upper threshold levels in the
instrument. The shaped signal input is split and routed through the two threshold circuits. If the signal
pulse height is of adequate height to pass through E, then it is routed to an anticoincidence circuit. If the
signal is also above the second threshold, it too passes to the anticoincidence circuit, where, upon arriving
within a certain time window Δt, the anticoincidence circuit blocks these signals from passing and no logic
output pulse is produced. However, if the signal passes above the LLD, but not the ULD, the anticoincidence
circuit is not activated, and a logic output pulse is produced. Hence, if the input pulse does not fall within
E and E + ΔE it is rejected. The number of passed signals equals the number of observed counts over a
range of energies ΔE to produce a differential result.
Many modern SCA units can be operated as either an integral discriminator or SCA. In integral mode,
the device window ΔE is completely opened while the LLD sets the discrimination threshold. When operated
as an integral discriminator, the NIM upper 10-volt limit usually applies. Also, many SCA units have two
scales, adjusted with a simple switch, with one window that opens to the maximum of 10 volts, and a smaller
window with finer resolution that is limited to 1 volt maximum. The reason for the finer window resolution
is to allow the experimenter to narrow the energy window with greater precision. A differential pulse height
spectrum can be formed by first setting the ΔE window at a desired channel resolution, and subsequently
taking measurements at increasing values of E in increments of ΔE from 0 up to 10 volts. Although
an educational exercise, the multichannel analyzer (latter section) has made this method of producing a
differential pulse height spectrum obsolete.
For most SCA units, the timing information is not accurately correlated to the input time of the pulse.
This timing discrepancy occurs, in part, because of the leading-edge timing method usually used to determine
when the signal pulse height surmounts the threshold. Unfortunately, this method suffers from so-called “time
walk,” because the pulse recognition time is dependent on the slope of the input pulse rise time. There are
special timing SCAs that use constant-fraction timing, a method that compensates for varying amplitudes
and ameliorates this timing shift and gives consistently better timing results. Timing SCAs are designed to
minimize timing shift and dead time for a variety of detectors, including NaI:Tl, Si, and HPGe detectors,
thereby allowing better system time resolution and higher counting rates.

16 Otherlogic systems include resistor-transistor logic (RTL), transistor-resistor logic (TRL), transistor-transistor logic (TTL),
complementary metal-oxide-semiconductor (CMOS), and emitter-coupled logic (ECL), all having specific voltage ranges for
lows and highs.
Sec. 22.3. Components 1197

22.3.4 Counters (Scalers) and Timers


A counter is used to tally the pulses that emerge from the discriminator or SCA unit. Historically, these
units were called “scalers”, mainly because their operation required a scaling ratio to tally the number of
pulses entering the device. The reason for this operation was that, at one time, electromechanical registers
could not keep up with the high rate of delivery from a counting system, capable of recording on average only
60 counts per second [Price 1964]. Instead, a “scale-of-2” was used where one output appears for two inputs.
A series of n units gives a dividing factor of 2n ; hence the instrument scales down the number of pulses to
manageable levels for the register. The result is an accurate tallying of the counts, giving the scaler the
ability to indirectly record thousands of counts per second. The resolving power of these systems determined
the count loss rate, manifested as another source of dead time. Other systems with “scale-of-10” were also
developed. The period of operation of a scaler was controlled with a separate timer unit. Overall, the name
“scaler” is historical, and modern digital electronic registers no longer use this scaling method to record
pulses. Instead, the more appropriate name is “counter”, and has been adopted as common nomenclature
for modern pulse recording units.
High speed counters with rates exceeding 100 MHz are commercially available. These units typically
operate with a string of decade counters. Each decade counter can record up to 10 inputs (in binary the
number is 1010). Upon reaching the binary number 1010, the counter is reset to zero while a pulse is
simultaneously delivered to the next decade counter in the chain, increasing the count by 1. On the second
decade counter, a binary number 1010 is then equivalent to 102 counts. Hence, a string of n decade counters
can register up to 10n counts before resetting. Commercial units commonly have 8 sequential decade counters
(an 8-decade counter).
The timer is used to start and stop the counter at preset time lengths. Usually the timer can be set
to count for a certain length of real time, where the counter only functions during the preset time interval.
Another timing mode feature allows a certain number of counts to be recorded, stopping to show the
lapsed time when a preset number of counts is reached. Many timers can be set to scroll, where after
a measurement period ends, there is a short delay before the tally is zeroed and another measurement
automatically commences.
Timing systems that use the power-line AC frequency as the clock work adequately well and are relatively
inexpensive, but they are best suited for use in countries that maintain power-line frequency corrections.
However, the actual AC frequency is averaged over a relatively long period of operating time, meaning that
short-term timing operations may suffer some inaccuracy. For short measurement time periods, seconds or
minutes for instance, a timer based on a crystal-controlled oscillator is preferred.
Depending on the application, counters can be acquired either as independent units, sometimes with
more than one counter in a single unit, or as combined counter/timer units having a built-in timer. Display
counters have a display for the counting operation, often an 8-digit digital display capable of handling
the maximum output from an 8-decade counter. The obvious convenience of a display counter is that the
operator can visually monitor the counting process during the operation. Blind counters do not have a
counting display, but instead can be interfaced with another display device such as a computer to log the
number of counts. In some counter/timer units, there is a display counter, but the timer is blind. Printing
counters, as the name implies, have an added capability that they can be connected to a printer to provide
an output. Overall, counters and timers can be acquired for various applications, and specification sheets
provided by manufacturers supply necessary information on maximum counting rates, display type, and
output type.
1198 Nuclear Electronics Chap. 22

22.3.5 Ratemeter
A ratemeter is another type of radiation pulse record-
Tw vin vout ing device that produces an output charge (or volt-
C1 small t age) proportional to the rate of radiation interactions
vo C2 R in the detector. This type of detector was intro-
large t
T duced by Gingrich et al. [1936] (see also Evans and
Alder [1939]). A ratemeter design in common use is
Figure 22.30. The basic diode charge pump ratemeter circuit.
a diode charge pump circuit [Vincent 1960; Vincent
and Parker 1970] and is depicted in Fig. 22.30. Con-
sider the input pulse train of square waves as shown in Fig. 22.30. Each pulse has voltage magnitude vo with
width Tw and period T . The capacitor C1 stores charge q1 with voltage v1 = q1 /C1 . The pulse input to the
diode charge pump causes the capacitor C2 to accumulate charge q2 , which discharges through the resistor
R with a time constant RC = τ . If the capacitance C1  C2 , then the charge passed to C2 is equivalent
to v1 C1 . The instantaneous output on the meter fluctuates in time, although it can be assumed that there
is an average input value. The amount of fluctuation about an average is a function of the time constant
τ , where a large value of τ decreases the fluctuation (less discharge) while a small τ has greater fluctuation
(more discharge).
In reality, radiation pulses arrive at sporadic intervals with varying amplitudes. Instead of a wave train,
what is actually observed are fluctuations in stochastic arrivals which contribute to the uncertainty in the
measurement. The total charge measured on C2 is q2 while each pulse produces an average charge of q̄. For
instance, recall that a Geiger-Müller counter produces pulses of nearly the same amplitude regardless of the
original particle type or energy. Given a fixed measurement time interval, the number of interacting particles
within that time period can be found from
q2
N= , (22.150)

with fractional standard deviation,
√ 
σN N 1 q̄
= = √ = . (22.151)
N N N q2
The standard deviation of the measured q2 is thus
σN √
σq2 = q2 = q̄q2 . (22.152)
N
The amount of charge on the capacitor C2 at t0 is the remaining amount after the prior charge input.
For an average charge q̄rdt produced between times t and t + dt, the amount of remaining charge on C2 is

t0 − t
q2 (t)dt = q̄r exp − dt (22.153)
RC2

where r is the average rate of particle interactions. The standard deviation of the charge is

σq2 = q̄ rdt, (22.154)

and, therefore, the contribution to the standard deviation at t0 is


√ t0 − t
σq2 = q̄ rdt exp − . (22.155)
RC2
Sec. 22.3. Components 1199

For all charge packages delivered to the circuit from the detector, the separate variances can be summed to
determine the total standard deviation
 t0
−2(t0 − t) q̄ 2 rRC2
σq22 = q̄ 2 r exp dt = . (22.156)
−∞ RC2 2
The average output current from the device is

ī = q̄r, (22.157)

while the instantaneous output current is


q2 (t)
i(t) = . (22.158)
RC2
Hence, with error propagation on Eq. (22.158) and substitution of Eq. (22.157) into Eq. (22.156), the variance
of the current is 
σq2 r
σi = = q̄ , (22.159)
RC2 2RC2
or the fractional standard deviation with respect to the average current (and also the counting rate) is

σi σr 1
= = . (22.160)
ī r 2rRC2
The average output signal is a function of the RC2 time constant. To understand this outcome, consider
the net rate of change on the capacitor C2 , where rq̄ is the charge rate and q2 /RC is the discharge rate
dq2 (t) q2 (t)
= q̄r − . (22.161)
dt RC2
Assuming at t0 = 0 there is no charge on C2 , then
 
−t
q2 (t) = rq̄RC2 1 − exp . (22.162)
RC2
Notice that as t becomes large (t RC2 )

q2 (t)  rq̄RC2 , (22.163)

which occurs at equilibrium. Hence, Eq. (22.156) and Eq. (22.163) are combined to find the average charge
output with standard error, 
rRC2
q2  q̄rRC2 ± q̄ (22.164)
2
or in terms of voltage 
q2 rR
vout =  q̄rR ± q̄ . (22.165)
C2 2C2
The output from a ratemeter can be altered by changing the RC2 time constant. A long time constant
RC2 provides a relatively steady output reading. However, the device takes longer to reach the equilibrium
condition and does not respond quickly to rapid changes in the count rate. Ratemeters accommodate different
count rates by making R adjustable. Modern instruments often have automatic meter ranging. To handle
large ranges of count rates, some ratemeters produce an output proportional to the log of the interaction
rate [for example, see Cooke-Yarborough and Pulsford 1951; Fraser 1974a, 1974b].
1200 Nuclear Electronics Chap. 22

22.3.6 Multichannel Analyzers


A multichannel analyzer (MCA) sorts shaped pulses from a linear amplifier according to their amplitudes.
The instrument operates by changing the analog signals from the amplifier into digitized outputs. By
digitizing and binning the pulse magnitudes, the resulting pulse height histogram produces a digitized image
of the differential pulse height spectrum. If analog signals are supplied to the MCA, then the instrument
must also incorporate an analog-to-digital converter (ADC). The analog-to-digital conversion architecture
affects both the speed and linearity of the system. Some types of ADCs are discussed below.
The ADC outputs are sorted by magnitude and assigned to channels divided equally by 2n over specific
voltage range, usually limited by the NIM maximum standard of 10 volts. For instance, the 10 volts may be
divided by 29 channels, yielding 512 consecutive channels each 19.53 mV wide. Most modern multichannel
analyzers allow the user to change the number of channels 2n from 256 up to 8192 by changing the value
of n. Hence, the multichannel analyzer17 operates, in some respect, as several SCAs sequentially scaled and
operating concurrently.
The MCA evolved over the last 70 years by incorporating many improvements. Early models used vacuum
tubes and, consequently, were quite large and were usually floor models. With solid-state electronics, these
devices were reduced to table top models with cathode ray tube screens and a pin-fed dot-matrix printer
readout. In the 1990s, the table top models were largely replaced by computer cards that would plug into a
PC bus. Although the computer card MCAs are still available through resale outfits, they have been largely
replaced by compact stand-alone units. Today, MCA instruments can be acquired as nuclear instrument
modules that insert into a NIM bin, or as independent portable units. User interface software allows the
operator to control the MCA and display the output on a personal computer or other electronic graphical
user interface.
The Analog-to-Digital Conversion
An analog-to-digital converter (ADC) is an electronic system that converts a continuous time and amplitude
signal into a quantized digital signal. For an MCA, the ADC converts an input analog voltage into a digital
output representative of the magnitude of the input pulse. An ADC system is limited by its bandwidth, i.e.,
by the maximum number of conversions per unit time that can be achieved. This limitation is a consequence
of the small time an ADC requires to process a conversion, a time in which additional signals cannot be
processed. Factors that affect ADC performance include sampling rate, aliasing, signal-to-noise ratio, jitter,
dither, linearity, and resolution, each of which is briefly described here.
The ADC resolution is determined by the number of discrete divisions spread over the analog voltage
range (or voltage span). These divisions are determined by the number of bits n. For example, an ADC
with n bit resolution over voltage span of Vm has channel resolution of,
Vm
ΔE = . (22.166)
2n
The actual resolution is limited by the signal-to-noise ratio, in which the noise consists of noise on the analog
signal and quantization noise. Electronic noise appearing with the input signal is also incorporated into the
digitized signal. Quantization noise appears as a consequence of the roundoff error between the analog signal
and the digitized result.
Linearity is important in spectroscopy measurements for accurate energy identification. The non-linearity
of an ADC is defined by either differential non-linearity or integral non-linearity. Differential non-linearity

17 At one time, multichannel analyzers were called “kick-sorters”, a term dating back to an electro-mechanical version of the
device that would project small spheres by way of an electromechanical plunger. The magnitude of the kick was proportional
to the pulse input, and the balls would land in a linear array of adjacent grooves to produce a histogram as the balls were
stacked. The device of Frank et al. [1951] had 30 channels (grooves), each capable of holding 100 balls.
Sec. 22.3. Components 1201

refers to the uniformity of channel widths ΔE defined by Eq. (22.166). The deviation in the width of MCA
channels is usually less than ±1% differential non-linearity for modern commercial instruments. Using a
linear fit for the channel assignment, the integral non-linearity refers to the maximum difference between the
original analog signal pulse height and the assigned digital channel as measured over the entire signal range.
For modern MCAs, integral non-linearity is usually on the order of or less than ±0.25% over the top 99% of
the dynamic range.
Dither refers to the process of adding white noise to the analog signal before digitization. The reason for
adding white noise is to improve the randomization of the quantization error, although such addition increases
the system noise. This method slightly extends the range of the ADC while smoothing the quantization error
over several noise values. Consequently, hard changes in digitized signals become smoother. Dither is widely
used in digital processing of audio and image data.
In many cases, the analog signal is continuous. Consequently, a method is required to measure the signal
and hold that specific value constant for a sufficient time to allow the ADC to produce a digitized output.
The process of holding the sampled signal constant is performed with a sample-and-hold circuit, in which
the sampled signal is used to charge a capacitor to store the charge. This capacitor is then temporarily
disconnected from the input while the signal is being digitized. The sampling rate is the average speed at
which an ADC can measure an analog signal (called sampling) to convert it into a digital output. This speed
is usually reported as “samples per second.”
To measure a periodic function, it is important that the sampling rate should be high enough to reproduce
an accurate representation of the original signal. Typically the sampling rate should be at least greater than
twice the analog signal bandwidth. A sampling rate that is too small can result in a problem called aliasing
in which the reconstructed input is no longer representative of the original periodic input frequency. Usually
a lower frequency digitized output is produced. The time between radiation pulses is stochastic, and the task
of the ADC is to measure and digitize the peak voltage of the shaped input signal. Related to sampling time
is the conversion time, defined as the time that it takes the ADC to sample an analog signal and process a
digital output. The ADC is essentially inactive to additional incoming pulses during the conversion process.
Hence, it is possible that these shaped pulses arrive at the ADC input faster than the ADC can process
them, which ultimately contributes to lost counts.
Jitter refers to the temporal uncertainty in significant events in the ADC process and is observed as
a deviation from the ideal timing interval between sampled signals. When the sample-and-hold circuit is
opened, the capacitor is connected to the input circuit and stores the signal. The clock closes the circuit
after some time Δt, while the ADC converts the stored voltage into a digital output. Jitter is the variation
in the time at which the switch is opened. Jitter contributes to uncertainty in the sampled voltage, and is
proportional to the amplitude and the rising edge of the input signal. Jitter problems increase with frequency
and pulse amplitude.

Stacked Discriminator
An ADC can be realized by combining a series of simultaneously operated SCAs. In this architecture, multiple
SCAs are arranged in parallel, each simultaneously accepting the shaped input pulse. Each separate SCA
defines a range ΔE, sequentially stacked over the entire acceptable input voltage range. This stack of SCAs
feeds a logic circuit that generates a code for each input channel. Ultimately, the stacked discriminator is
a fast method to digitize pulses, mainly because the output is routed to the correct accumulator in a single
step. Consequently, these ADCs are also called flash ADCs for their high speed capability. However, this
architecture is too expensive for modern MCAs with large numbers of channels. For instance, the number
of ADCs is equal to the digital resolution, which for an MCA with n-bit resolution requires 2n comparators.
Flash ADCs are usually restricted to 8 bit or to MCAs with only 256 channels. Also, the differential non-
linearity is sometimes a problem because the independent threshold values of voltage for each channel have
1202 Nuclear Electronics Chap. 22

their own associated error and, thus, add variance to the channel widths. Other problems include higher
input capacitance than other architectures, higher power consumption, and generally lower energy resolution
because of the restricted number of channels.
Wilkinson ADC
Introduced in 1950 [Wilkinson 1950], the Wilkinson
clock ADC is still one of the most popular architectures used
clock pulses
gate opens
in MCAs. An input voltage into the Wilkinson ADC
hold charges a capacitor while a voltage comparator is used
to monitor the charge. When the input capacitor volt-
input pulse height

capacitor age is equivalent to the magnitude of the input voltage,


voltage clock
gate closes the capacitor is discharged at constant current through
a linear network. Hence, the capacitor voltage decreases
input in time with a constant slope as shown in Fig. 22.31. By
pulse measuring the time it takes to fully discharge the capac-
itor, a relative measure of the original voltage is found.
time
This discharge time is determined by introducing a gate
Figure 22.31. Principle of the Wilkinson ADC operation. pulse when the capacitor begins to discharge. The gate
After Nicholson [1974]. pulse opens a linear gate that passes pulses produced by
a precision oscillator to act as a clocking timer. The gate closes when the capacitor is fully discharged.
While the gate is open, a discrete number of pulses is allowed to pass; hence the number of clock cycles
that pass through the gate is a digitized indication of the initial input pulse. These clock cycles are counted
on a digital address register. To prevent ambiguities in channel assignment, steps are taken to prevent the
discharge process from starting in the middle of a clock cycle [Nicholson 1974]. Because the ADC method
relies on a time-correlation, it becomes clear that large input pulses take longer to process than small input
pulses. Further, the processing time, which depends on the clock frequency, becomes smaller as the clock
frequency is increased. Commercial MCAs can be acquired that operate linearly with clock frequencies on
the order of 100 MHz.
Successive Approximation ADC
A successive approximation ADC uses a comparator
1st 2nd 3rd 4th 5th 6th
and a successive binary approximation method (see
E stage stage stage stage stage stage Fig. 22.32). An input shaped voltage pulse is initially
compared to a range determined by E/2, where E is
the maximum range of interest. For example, E might
V correspond to the NIM standard of 10 volts. If the
input voltage V is larger than E/2, then a ‘1’ is gen-
erated in the output, and the difference V − E/2 = V1
E/2 is passed to the next stage. If, instead, V is less than
E/2, then a ‘0’ is assigned and V = V1 is passed to
the second stage unaltered. At the second stage, the
E/4
process is repeated, except the comparison is now per-
E/8 formed between V1 and E/4. Hence, if V1 is greater
input E/16 E/32 than E/4, then another ‘1’ is assigned and V1 − E/4 is
pulse
passed. If V1 is instead less than E/4, a ‘0’ is assigned
1 0 1 1 1 and the unaltered signal is passed. This process con-
Figure 22.32. Principle of the successive approximation tinues through a series of binary comparisons until the
ADC operation. After Nicholson [1974]. channel limit is reached. Hence, with 2n channels for
Sec. 22.3. Components 1203

the MCA there are n comparison stages. Each result is stored in a successive approximation register. The
final output is the binary number representative of the digital conversion of the analog signal. The main
advantage of the successive approximation register is that each input pulse takes essentially the same amount
of time to process, which is usually less than that required for large pulses in a Wilkinson ADC in an MCA
having a large number of channels. Hence, the successive approximation ADC is potentially faster than the
Wilkinson ADC.

Ramp-Compare ADC
The ramp-compare or digital ramp ADC introduces a saw-tooth ramp input signal that is incremented by
a counter. The ramp is produced by initiating a digital counter that has its output tied to the input of
a digital-to-analog converter (DAC). This DAC ramp output is compared sequentially at each step to the
amplitude of the shaped input voltage. The first comparison is performed with the ramp voltage at zero.
If the input voltage is higher than the DAC signal, then the comparator produces a ‘1’ which signals the
counter to increment by one. The DAC output is therefore also incremented by one voltage division and
the comparison is repeated. When the DAC output signal matches the shaped input signal, within a set
division tolerance, the counter transfers the binary number to a shift register, and the comparator indicates a
match and resets the counter to ‘0’. The shift register transfers the binary count to the ADC circuit output.
Unfortunately, these ADCs are relatively slow and sensitive to the thermal changes. Further, their output
speed is a function of the initial input pulse height because it takes longer to process the signal as the pulse
height increases.

Sliding Scale Smoothing


A problem arises from the variance in channel widths of an MCA, where some channels are given more weight
than others. This variation in channel width ultimately skews the digitized pulses that accumulate in each
channel. For instance, pulses of a particular range falls between two levels that mark a channel width. If that
channel width is wider or narrower than the average, then the number of pulses assigned to that channel is
greater or smaller than the average. The variance and linearity of an ADC can be improved by a technique
introduced by Cottini et al. [1963], known as sliding scale smoothing. The method alters the shaped input
pulse before digitization, returning to its former value afterwards by the following sequence. The analog
input pulse V has an analog value Ei added to it. After running through the ADC, the digital value of Ei
is subtracted, ultimately returning to the digital value of V . However, the value of Ei is randomized over
various i, meaning that the assigned values after digitization also vary. With subtraction of Ei , the process
produces an average value spread over a few channels and, thereby it ameliorates the influence of channel
width variance.

22.3.7 Pulse Generators


An important electronic component that assists with calibration of the radiation counting system is the
pulse generator, which is commonly referred to as a pulser. Pulsers provide accurate voltage test pulses into
the radiation detection system. The pulses can be set to have different shapes (a tail pulse being the most
common), decay times, pulse frequencies, and amplitudes in order to calibrate an amplifier, MCA, SCA, or
counter/timer. The test pulses can also be used to help determine system dead times and system electronic
noise. Although not necessary to operate a radiation counting system, they are quite valuable when first
configuring the system and calibrating it for radiation measurements. Further, a pulser is usually operated
during a spectroscopic measurement in order to have a comparison peak with which the system noise can be
determined. Typically the pulser peak is set to an MCA channel that does not interfere with the accumulated
radiation spectrum. Some vendors offer digital pulsers with multiple pulser outputs.
1204 Nuclear Electronics Chap. 22

22.3.8 Power Supplies


Detectors that operate with the NIM system typically produce an electronic output and, therefore, require
a power supply of their own. Traditionally, the majority of such NIM power supplies for detectors apply a
high voltage to the detectors. Stability of the supply voltage is of particular importance in high-resolution
spectroscopic systems. High-voltage power supplies are used to operate detectors that do not suffer changes
in capacitance as a function of voltage, such as gas-filled and scintillation detectors. High-voltage bias power
supplies are usually used for semiconductor detectors, in which the operating voltage can affect the detector
capacitance.
High-Voltage Power Supply
The high-voltage power supply, as the name implies, supplies high voltage to the detection device, and can
supply it with either positive or negative polarity. The voltage is applied to the detector across a load resistor
with the connection routed through the preamplifier unit. Typically, a power supply has a meter indicating
the applied voltage and it is reasonably accurate because the detector resistance is usually much greater than
the preamplifier load resistance. HV power supplies are available with the maximum voltages exceeding 3.5
kV. Such units are commonly used with PMTs and gas-filled detectors, neither having capacitance changes
as the applied voltage is varied. As discussed in Sec. 14.1.6, a small change in output voltage can produce
a large change in a PMT output. Consequently, power supplies used for scintillation spectrometers require
high-voltage regulation to prevent voltage drift. Commercial units quote stability specifications as usually
less than 0.03% variation over a 24-hour period. Also, because PMTs require high voltage to operate and
often with current in the mA range, a HV power supply is usually connected directly into an AC receptacle.
For convenience, many models have rails that allow the unit to slip into a NIM bin compartment.
High-Voltage Bias Supply
For semiconductor detectors, the power supply is generally referred to as a “bias supply.” As with a HV
power supply, the bias supply provides a choice of positive or negative high voltage to the detector. However,
this type of power supply usually does not have a meter, but rather only a dial indicator indicating the total
applied voltage to the system. Because the system includes load resistances in series with the detector, there
is a voltage drop across this resistance, which reduces that applied to the detector. Thus, a meter indicating
total voltage would be misleading. Instead jacks are often provided that allow determination of the bias
current. Because the series’ load resistance is known, the voltage applied to the detector, which is less than
the total, can also be determined by subtracting iR from the overall applied voltage. Bias supplies are
available for which the maximum allowable voltages can exceed 5 kV. Because typical detectors are highly
resistive and draw little current, the power requirement of the bias supply is low and, consequently, most
bias supplies are connected directly into the NIM bus for power, unlike HV power supplies. Stability in
commercial units is commonly quoted as less than 0.1% variation per hour.
NIM Power Supply
A power supply is attached behind a NIM bin to supply power to the modules. This unit provides ±6
volts DC, ±12 volts DC, and ±24 volts DC to the NIM sockets and voltage jacks,18 as well as 117 volts
AC. Power is commonly rated between 150 and 160 W for the larger power supplies, although lower power
models rated at about 95 W are available (usually for models that do not offer the ±6 volt DC option). The
NIM bin sockets and pin assignments conform to the specifications outlined in DOE/ER-0457T. Test jacks
in the front of the NIM bin provide convenient access to monitor the DC voltage, and can also be used to
conveniently supply power to custom electronics. Modern power supplies are filtered from electromagnetic
interference (EMI), are short-circuit proofed, thermally protected, and provide stable power required for

18 Some models do not provide ±6 VDC.


Sec. 22.4. Timing 1205

V(t) 2st V(t)


(a) (b)

VT 2sn

2
VT

T time DT time

Figure 22.33. The effects of (a) time jitter and (b) time walk on the timing uncertainty,
where VT is the timing trigger threshold.

NIM components. Usually NIM bins have warning indicators that inform the operator if the power supply
is approaching the temperature limit.

22.4 Timing
Sometimes it is important to know the time a radiation pulse occurs. Examples where such timing in-
formation is needed include coincidence measurements, anticoincidence measurements, and time-of-flight
measurements. Timing systems use comparator circuits to determine the time at which a pulse amplitude
reaches a preset threshold and then produce a logic pulse at the moment the pulse crosses the threshold.
This logic pulse can then be used as a synchronization signal for timing measurements.

22.4.1 Jitter and Time Walk


Jitter refers to noise variations on the input signal as shown in Fig. 22.33(a). Consider a threshold voltage
denoted VT used to trigger a time stamp on an incoming pulse. The average value of an input pulse v(t) is
depicted as the dotted line in Fig. 22.33(a). However, electronic noise causes a variance in the time dependent
input signal at VT . This variance is quantified by the standard deviation σn of the noise. This variance in
noise causes a variance in the actual time that the signal passes the threshold VT and is quantified by the
standard deviation σt . Because of these variances, there is uncertainly in the time stamp due to the jitter.
Note that σn is simply the voltage amplitude of the noise. The contribution of the noise to the timing jitter
is represented by [Spieler 2005] & 
dV 
σt = σn . (22.167)
dt  VT

If the noise cannot be reduced, the jitter can still be minimized by setting the threshold VT at the point of
the maximum slope of the input pulse.
For some timing methods, the amplitude of the input pulse causes changes in the trigger time. Consider
the leading edge of two analog pulses of different amplitude as depicted in Fig. 22.33(b). Both pulses start
at the same time and are triggered at the same threshold VT . For the larger amplitude pulse (1), the pulse
crosses VT before the smaller pulse (2). The difference ΔT in the trigger time is called time walk. The
trigger timing of pulses shifts with pulse height and, thus, contributes to the uncertainty of the trigger time.
Time walk can also appear as a consequence of different rise times, even if the pulse amplitudes are identical.
For instance, the pulse output is a function of the location of radiation interaction in a HPGe detector (see
Sec. 16.4.2), and these different rise times cause the trigger time to change. Time walk exacerbates the
effects of jitter on the timing uncertainty. Some systems may partially compensate for time walk by making
1206 Nuclear Electronics Chap. 22

appropriate corrections from the slope of the pulse. However, such methods reportedly fail if the input pulses
suffer time walk from both amplitude and rise time variances [Spieler 2005]. Otherwise, time walk can be
reduced by setting VT at the lowest possible setting without being triggered by noise. Unfortunately, the
optimum settings for time walk and jitter are usually not at the same VT .

22.4.2 Common Timing Methods


There are many methods for recording the arrival time of pulses, and choosing the appropriate method
should include consideration of the required timing resolution and type of detector in use. Briefly outlined
in the following sections are a few popular methods of recording pulse arrival times.
Leading-Edge Timing
The leading-edge triggering method is relatively straightforward, and used when timing information is needed
with somewhat relaxed timing resolution. The operator can set a threshold VT and a comparator circuit
identifies when the time dependent input pulse matches this preset threshold, at which point a logic pulse is
generated. Some units provide a preset logic pulse length, while other units may terminate the logic pulse
when the falling slope of the pulse once again matches VT . However, leading edge timing is susceptible to
resolution degradation from time walk and jitter. Nicholson [1974] reviews a few select designs for leading
edge timing trigger circuits.
Zero-Crossover Timing
If the input signal is converted into a bipolar pulse, then the zero point crossing of pulses with varied
amplitudes is time-invariant as shown in Fig. 22.34. Consider the result of a CR-RC shaping network from
Eq. (22.107). Adding a differentiator (as in Fig. 22.13) produces a bipolar output
d d t −t/τ τ − t −t/τ
Vbp = Vout = Vin e = Vin e . (22.168)
dt dt τ τ2
From this result it is seen that the output becomes zero when t = τ . Note that the zero crossing is only a
function of the shaping time and not the amplitude. Zero-crossover timing is best used for detectors that
produce a wide range of pulse amplitudes.
Such a system can be set to trigger when the zero-crossover condition
V(t)
1 is met, ideally eliminating problems with time walk. Noise can also trig-
ger the timing circuit when noise pulses cross the zero point. To prevent
confusion between noise and radiation pulses, a leading edge threshold
comparator is often included to discriminate against noise. The original
2
pulse is split and passed through both the threshold comparator and the
VT zero crossover network. If the original pulse triggers the threshold com-
time
parator, indicating that the pulse is real and not noise, a signal is sent to
an AND gate19 that temporarily allows signals to pass. If both signals
arrive in coincidence at the output gate, then a logic pulse is generated.
Otherwise, the zero crossover pulse is blocked. The circuits are generally
engineered such that the discriminator comparator signal is stretched and
arrives at the gate before the zero crossover signal, thereby synchronizing
Figure 22.34. The zero-crossover the time signal with the arrival of the zero crossover time signal.
timing method. There are a few problems associated with the zero crossover method.
First, with any timing circuit, there is a small delay from the time that the trigger condition is met and

19 AnAND gate is a digital logic gate that produces a “high” output (or 1) only when all inputs are also “high”. Otherwise, the
output is “low” (0).
Sec. 22.4. Timing 1207

V(t)
-fV 1
-V

-fV 2

fV 3

Dt

4
0
time
td

Figure 22.35. Constant fraction timing method. The inverted nega-


tive input (1) is reduced by fraction f (2). The input pulse is inverted
and delayed by Δt such that a fraction of the input pulse f V equals the
attenuated pulse maximum (3). Adding (2) and (3) together causes
(4) the summed pulse to cross zero at the delay time td .

when the comparator initiates the trigger. Hence, there is a small amount of time walk. Second, the zero
crossover point can shift with pulses of different rise times and shapes, such as those produced by HPGe
detectors. Finally, jitter can be worse for zero crossover timing than leading-edge timing [Nicholson 1974].
For detector measurements where the pulse amplitudes are similar, the time walk may be less of an issue
than jitter, and leading-edge timing may be a better choice.

Constant Fraction Timing


Another method developed to reduce the effect of pulse height time walk is constant fraction timing, which
also uses a zero crossover method [Gedcke and McDonald 1967; 1968]. The input pulse V is split and one
branch is attenuated by a fraction f of the pulse amplitude, while the other branch is inverted and delayed.
The fraction f can be chosen to minimize jitter.
The delay time Δt is chosen to shift the rising edge of the inverted input pulse, the location at f V , to
align with the maximum of the attenuated pulse, which is also f V (see Fig. 22.35). The delayed inverted
pulse is added to the attenuated pulse, which produces a bipolar pulse that crosses zero at the time denoted
td . A logic pulse is generated when the bipolar pulse matches the zero condition. The end result is a timing
method that no longer suffers from amplitude time walk. This method is also less affected by time walk due
to variations in rise time than is the leading edge method [Ortec 2009c]. Further, for relatively low values of
f (less than 0.4), the timing resolution remains relatively constant.

ARC Timing
The amplitude and rise time compensated (ARC) timing method was developed for detectors that produce
pulses that vary in rise time and pulse amplitude, which is particularly true for HPGe detectors [Chase 1968;
1208 Nuclear Electronics Chap. 22

Cho and Chase 1972]. From the explanation for time-dependent pulse height formation in a planar HPGe
detector given in Sec. 16.4.2 and shown in Fig. 16.31, the pulse rise takes on various shapes as also shown in
Fig. 22.36.
V(t) The ARC timing method has some similarities to the constant frac-
er

tion timing methods. The input pulse V is split, where one branch
ent

is inverted and attenuated by a fraction f of the pulse amplitude,


or c

n ds
re
and the other branch is delayed by Δt and then added to the attenu-
ect

c to ated pulse. The summed signals produce a bipolar pulse with a zero
det

te
de crossover that triggers a logic pulse. The main difference from con-
stant fraction timing is that the delay Δt is chosen to be small. From
time Fig. 22.36, pulses from a planar semiconductor detector are initially
Figure 22.36. Position-dependent pulse
linear. Once one type of charge carrier is collected (holes or electrons),
shapes for a planar semiconductor detec- the pulse shape changes to have a slower rise. ARC timing has time
tor. If the charge speeds are equal, the walk if the slope changes before the zero time crossing. By choosing a
shortest rise time is for events occurring small Δt to delay the pulse, the zero crossover occurs before the pulse
at the center of the detector because both
electrons and holes are collected at the becomes non-linear, and consequently is independent of the overall
same time. The longest rise times occur rise time and pulse amplitude (see Fig. 22.37). As with the bipolar
when events take place at the ends of the and constant fraction timing methods, a threshold comparator is used
detector. to remove zero crossings caused by noise pulses.
The ARC timing method has been shown to work well with coaxial HPGe detectors [Cho and Chase
1972]. However, the slope of pulse shapes from coaxial detectors is non-linear, changing between a mix of
convex and concave shapes depending on interaction location (see Fig. 16.32). Consequently, ARC timing
does not completely eliminate time walk with coaxial detectors, although it does show better performance
than most other timing methods.
Some coaxial HPGe detector pulses can have relatively long rise times, generally caused by the excitation
of electron-hole pairs in a region with low electric field, thereby initially producing low carrier speeds. If the
discriminating comparator fires relatively late because of a slow rising pulse, then the gate is closed when
the zero crossover signal arrives. Instead, the gate is opened late, corresponding to the arrival of the leading
edge trigger instead of the zero crossover time. Consequently, these pulses can cause time walk that severely
distorts the time spectrum. To counter the effect, slow rise time (SRT) rejection can be used to block the
timing output if the zero crossover signal arrives before that of the leading edge discriminator signal [Bedwell
and Paulus 1976].

22.5 Coincidence and Anti-Coincidence


There are many applications that require the measurement of coinciding events that occur in two or more
separate detectors within a specified time interval. Examples include identification of the simultaneous
arrival of photon-photon or photon-particle events, applications involving positron decay, and determination
of radioactive decay schemes. Such measurements are commonly referred to as coincidence measurements,
in which two or more events are considered coincident if they arrive at the coincidence discriminating unit
within a preset time window of width τ . Accuracy of these measurements depends on the time correlation
of the events that depends on a time window which must be set large enough to identify coincident events
while being narrow enough to exclude uncorrelated events.
For example, positron emission tomography (PET) seeks to correlate annihilation photons from a single
positron decay event and usually is based on the photons entering separate pairs of detectors arranged 180◦
about the source. Coincidence measurements can also be used to characterize light yield in scintillators, as
explored by Rooney and Valentine [1996]. Coincidence counting is also used to distinguish between radiation
Sec. 22.5. Coincidence and Anti-Coincidence 1209

V(t)

V 1

-fV
2

1-fV 4
0
crossover
time
Dt
Figure 22.37. The ARC timing method. The input pulses (1) may have different
rise times, depending on the interaction location. An input pulse is split into two
signals, where one input pulse is inverted and reduced by fraction f (2). The other
input pulse (3) is delayed by Δt, starting at only a small fraction of the rising
pulse. Adding (2) and (3) together causes the summed pulse (4) to cross zero at
the same delay time, regardless of rise time or pulse height.

types, for example the selective imaging of beta particles that are coincident with gamma-ray emissions
[NCRP 1985; Dewaraja et al. 1994].
By contrast, there are some measurements that require the opposite condition, i.e., when two radiation
events are recorded within time interval τ are rejected. Such measurements are referred to as anticoincidence
measurements. For example, Compton suppression spectroscopy is a measurement method that uses the
technique of anti-coincidence [Lindblad 1978; Bender et al. 2015] to reduce the Compton plateau in a pulse-
height spectrum.

22.5.1 Coincidence Analyzers


The main function of a coincidence analyzer is to discern the arrival of two or more radiation particles in
separate detectors within some preset time interval τ . In practice, it is not possible to analyze coincidence
events with 100% confidence due to the uncertainties associated with the statistical nature of radiation
emissions. Statistical timing errors may occur from the detection process and uncertainties in the electronics
resulting from timing jitter, amplitude walk and noise, all of which lead to statistically variable time delays
between processed events.
A coincidence analyzer accepts the time stamped inputs from two or more detectors, each connected to
a separate port. Input signals are converted into stretched logic pulses, where the time duration is set to τ .
A simple coincidence circuit solves this problem by essentially summing the two input pulses, passing the
resultant sum pulse through a discriminator level, and generating an output pulse when the summed input
pulses exceed the discriminator setting.
The period of time in which the two input pulses can be accepted is defined as the coincidence resolving
time τ . Commercial coincidence modules allow the user to set τ within limits, usually between tens of ns up
1210 Nuclear Electronics Chap. 22

to a few μs. A time-stamped pulse enters one port of the unit. If during the set resolving time another pulse
enters another port of the unit, it is considered coincident. It does not matter which signal arrives first. If
both signals overlap, then the coincidence analyzer produces an output logic pulse. Commercial units also
often have an anti-coincidence feature in which, by either flipping a switch or connecting an input to an
anti-coincidence port, logic pulses are generated at the output only if pulses are not coincident.
Suppose an input pulse arrives at a random time t1 . It is possible that a pulse already arrived at port
2 between time t1 − τ , causing a coincidence. It is also possible that a pulse arrives at port 2 between
time t1 + τ , also capable of producing a coincidence signal. Consequently, the actual window for possible
coincidence is the sum of these two intervals, namely 2τ . Because detector events occur at random times,
accidental coincidences can occur between two pulses which produce background in the coincidence counting.
Suppose that two counting rates are recorded by two separate detectors. The experimenter would observe,
on average, g1 cps from detector 1, about which for any single count a coincidence may arrive within ±τ .
The average number of counts recorded from detector 2 within the time window is g2 (2τ ) so that the average
rate of accidental or random coincidences is

ga = g1 g2 (2τ ). (22.169)

For N -fold detectors, the accidental coincidence rate is determined as [Jánossy 1950],

ga = N g1 g2 . . . gN τ N −1 + higher order terms. (22.170)

For the case where ni  τ , Jánossy [1950] shows that the higher order terms are negligible, yielding [Fenyves
and Haiman 1969],
ga  N g1 g2 . . . gN τ N −1 . (22.171)
Consider a two-fold coincidence system where detectors 1 and 2 have counting rates g1 and g2 , respectively.
If the source activity S is known and the source is relatively small, the count rates recorded by each detector
are
gi = Si Ωf i Bi i = 1, 2, (22.172)
where for the ith detector Bi represents correction factors (such as the source branching ratio), Ωf i is the
fractional solid angle subtended by the detector from the source, and i is the detector counting efficiency for
the radiation of interest and source location. The rate of true coincidences depends upon the source activity
S and the probability that concurrent emissions arrive at the detectors with respect to the source-to-detector
solid angles,
gt = S(1 Ωf 1 B1 )(2 Ωf 2 B2 ). (22.173)
The accidental coincidence rate is the detection rate of uncorrelated emissions. From Eq. (22.171), the
accidental coincidence rate is
ga = 2τ S 2 (1 Ωf 1 B1 )(2 Ωf 2 B2 ). (22.174)
The ratio of Eq. (22.174) to Eq. (22.173) yields
ga
= 2τ S, (22.175)
gt
which shows that the ratio of accidental to true coincidences increases linearly with source activity and
resolving time. Note also that the source activity can be determined by dividing Eq. (22.175) by the value
of 2τ .
The number of counts recorded by the detectors depends upon the experimental geometry and the
detectors used. A good method to reduce accidental coincidences is to make the resolving time as small as
Sec. 22.5. Coincidence and Anti-Coincidence 1211

possible. However, the resolving time cannot be better than the system time resolution, which is affected by
jitter and time walk. Consequently, the timing methods and detector types together determine the limitations
on the resolving time. The limited resolution is depicted in Fig. 22.38(top), where the coincidence count
rate is shown as a function of count rate (a differential
time spectrum). Given identical equipment with iden- dr true 2t 2t
dt coincidence
tical delay times between the detectors and the coinci- a
peak
dence analyzer inputs, both pulses should arrive at the
coincidence analyzer at identical times. In other words,
if one pulse arrives at t1 , then the other pulse should
accidental
also arrive at t1 , although the arrival times may instead coincidences
be slightly different because of jitter, time walk, and
ta

coincidence count rate


perhaps other effects. Without this deviation, the co- 2t
incidence peak would be represented by a single chan- ideal
true
nel; however, in reality it is statistically spread out coincidences
resolution
over several channels. limited
Typically, the detectors and electronics for each de-
tector branch are different. Suppose that a resolving accidental
time τ is selected that is wider than the actual coin- coincidences

cidence peak, as depicted in Fig. 22.38. If the arrival ts tv


time of one coincidence pulse arrives at time ts , then
a coincidence from the other pulse is logged provided Figure 22.38. (top) The expected differential time spec-
trum for coincidences, where r is the coincidence count rate,
that it arrives within ts ± τ . A delay line on each ts is the set arrival time at one input, and ta is the variable
branch of the circuit, depicted in Fig. 22.40, allows arrival time at the other input. (bottom) The coincidence
the user to set one delay time ts while also varying count rate observed from a coincidence analyzer with re-
the other delay time, denoted by tv . The operator can solving time τ and variable delay input tv .
then take coincidence measurements at different values of tv , thereby producing an output response as shown
in Fig. 22.38(bottom). If the delay is too small, such that tv < ts −τ , or if it is too large, such that tv > ts +τ ,
then any coincidence measured is accidental. If the delayed pulse arrives such that ts − τ < tv < ts + τ , then
real coincidences are tallied along with accidental coincidences. Hence, by setting the variable time delay tv
in the center of the delay curve spectrum, the operator measures the sum of true and accidental coincidences.
The true coincidence rate is determined by subtracting the accidental count rate of Eq. (22.169).
The coincidence count rate increases as τ is increased, mainly be-
cause the accidental coincidence rate increases. The coincidence ana-
coincidence count rate

lyzer output can be optimized by measuring the delay curve response as


2t1
a function of both τ and tv , as depicted in Fig. 22.39 [Nicholson 1974].
1
If τ is longer than needed, the delay curve has a flat top response,
shown as (1) and (2) in Fig. 22.39. If τ is too narrow, true coincidences 2t2
are rejected and the count rate maximum incorrectly reports the coin- 2
cidence rate, depicted as (4) in Fig. 22.39. However, at the optimized 2t3
τ setting, there is no flat top to the delay curve ((3) in Fig. 22.39), and
3
the peak location correctly indicates the sum of the true and accidental
4 2t4
coincidence rates. Notably, the delay tv must equal ts for the optimized
condition. The advantage of narrowing τ to the optimum value is the ts tv
reduction of background accidental coincidences.
Figure 22.39. Depiction of delay
Consider the timing analysis system depicted in Fig. 22.40. Two curves for various values of the coin-
detectors are positioned to measure coincident events from a radiation cidence resolving time τ , showing the
source. These coincidences may include, for example, positron annihi- sum of real and accidental coincidences.
1212 Nuclear Electronics Chap. 22

delay
line

timing gate
preamplifier amplifier delay 1
discriminator
detector MCA

coincidence counter/
source
analyzer display

detector
timing
preamplifier amplifier delay 2
discriminator

Figure 22.40. A method of using a coincidence analyzer for measuring coin-


cident events.

lation photons, dual gamma-ray emissions such as those from 60 Co, and beta particle/gamma-ray coincident
events. The selected detectors should detect the radiation emissions of interest with good efficiency and/or
energy resolution. They need not be the same type of detector. For instance one detector may be a NaI:Tl
detector. while the other is an HPGe detector. The HPGe detector can be used for its excellent energy res-
olution while the highly efficient scintillator provides the coincidence signal. The signals are passed through
preamplifiers and amplifiers compatible with the timing requirements. The time stamps for pulses from
either detector are produced by a timing discriminator that uses one of the timing measurement methods
previously discussed. The pulse processing chain from the separate detectors may cause coincident events
to emerge from the timing discriminators at different times. If so, this problem is remedied by placing a
variable delay instrument after the timing discriminator. Although Fig. 22.40 depicts a delay after each
timing discriminator, often one delay line or delay amplifier placed on the faster processing chain is adequate
to synchronize the pulses as they converge on the coincidence analyzer. If counting coincident events is all
that is required, the signals from the coincident analyzer can be routed to a counting system. If the goal
is to produce a pulse height spectrum from the high resolution detector only of the coincident events, then
the signal from the amplifier can be split and routed to the coincidence analyzer and also into another delay
module. If a coincidence is triggered, the logic pulse opens a gate that allows the high-resolution detector
pulse to be logged by a multichannel analyzer. The delay on the high resolution pulse is set to arrive within
the time that gate is open.

22.5.2 Time-to-Amplitude Converter


The time-to-amplitude converter (TAC) is a measurement module that converts the difference in arrival
times between events into a histogram, much like a pulse height spectrum. However, the abscissa is in units
of time rather than energy. The timing resolution is defined as the full width at half maximum (FWHM) of
the pulse height spectrum. The device operates by accepting a start signal and a small time later accepting
a stop signal. Unlike the coincidence analyzer, the order that pulses arrive at the input does matter. A delay
is at times employed to ensure that the stop signal arrives at some time Δt behind the start signal. These
signals can be provided by separate detectors whose pulses have passed through a timing discriminator,
perhaps timed with one of the methods previously described.
The circuit is arranged with a constant current source supply that is routed through start and stop
switches. These switches are initially in the closed position, which normally routes the current to ground.
The start switch is also in parallel with a converter capacitor that is tied to an amplifier input. When the
leading edge of the start signal arrives, the start switch is opened which then allows the constant current
source to charge the converter capacitor. When the leading edge of the stop signal arrives, the stop switch
Sec. 22.5. Coincidence and Anti-Coincidence 1213

is opened to disconnect the constant current source from the circuit. The charging current produces the
voltage
iΔt
V = , (22.176)
C
where i is the constant current, Δt is the time spacing between the start switch opening and the stop switch
opening, and C is the converter capacitance. Hence, the stored voltage is a linear measurement of Δt.
Shortly after the stop switch opens, the voltage in the form of a square wave is passed through a linear
gate to an amplifier and to the TAC output. The amplitude of the output is indicative of time Δt, which
can be supplied to a tallying unit such as a multichannel analyzer. Shortly thereafter, the switches are
closed and the converter capacitor is discharged to ground, thereby resetting the circuit for the next timing
measurement.
The use of a TAC can greatly simplify a coincidence mea- MCA MCA
surement system. The TAC timing method eliminates the need channels channels
true (window 1) (window 2)
to produce a delay curve, and there is no need to set a resolving

counts per channel


time. The logic signal amplitudes produce a pulse height spec-
FWHM
trum in which the pulse height is a function of Δt. Hence, the
spectrum directly yields the time resolution of the system. The
channels have units of time so the channel resolution (time per
accidental accidental
channel) can be changed by varying the conversion gain of the
MCA. A TAC coincidence spectrum is depicted in Fig. 22.41. time
The time resolution is measured by the FWHM of the true
Figure 22.41. Depiction of an MCA spectrum
coincidence peak. Shown is a window about the coincidence provided by a TAC coincidence system.
spectrum where the total counts in the window are the sum of
true and accidental coincidences. The net true counts can be determined by setting a window of equal width
(channels) away from the peak, and subtracting the counts in the second window from the counts in the first
window.
One possible arrangement using a TAC is depicted in Fig. 22.42. The system is fundamentally similar
to the system of Fig. 22.40, but a single delay line is used to ensure that the stop signal arrives after the
start signal. The output of the TAC is a function of the time difference, thereby delivering a differential
time spectrum to the MCA. Because the logic pulse amplitudes from the TAC are a function of the Δt, the
difference between the start and stop times, the MCA produces a histogram of pulse height frequency as a
function of Δt.
Without noise or jitter, the TAC output would deliver a Δt output that is exactly the same for each
true coincident event. Hence, the differential time spectrum would fall into a single channel. Yet, this ideal
behavior does not occur. Because of timing variations due to jitter and time walk, there is an inherent

preamplifier amplifier timing


discriminator
detector

source TAC MCA

detector
amplifier timing
preamplifier delay
discriminator

Figure 22.42. A method of using a TAC for measuring coincident events.


1214 Nuclear Electronics Chap. 22

limitation to the time resolution. This resolution can be measured by connecting the TAC inputs to a single
detector or to a pulse generator. If the signal is split and routed through the two system branches and into
the TAC, it is expected that the output would have constant amplitude at some time T . The distribution of
pulses about this value of T renders a spectrum that includes the variance in Δt about T . The FWHM of
this differential time spectrum is commonly called the timing resolution. It is worth noting that the delay
shown in Fig. 22.42 is important. Without the delay, the true coincidence spectrum would be centered about
T equal to zero. pulses occurring at T − Δt would yield a negative output and thus not be counted.

22.6 Instrumentation Standards


Early nuclear instruments used vacuum tube circuits within a standardized 19-inch wide chassis. The
components each had their own DC power supply connected directly to AC power. These components,
which were easily installed in a standard 19-inch wide instrument rack, could be easily interchanged because
each unit operated independently.
The invention of the transistor in 1948 led to more compact electronics, which generated far less heat than
vacuum-tube components. Yet, these early transistorized nuclear instruments were built in a similar fashion
to their vacuum-tube counterparts and were still designed for large 19-inch wide racks. It was eventually
realized, however, that these transistorized electronic components could be built as smaller and more efficient
modular units, thereby eliminating the need for a single 19-inch wide chassis. Many independent laboratories
and commercial companies began to design and construct systems of various modular electronic components.
Two such systems, advanced at the time, were the systems developed by the European Organization for
Nuclear Research (CERN) and the United Kingdom Atomic Energy Research Establishment. The European
Standards community on Nuclear Electronics (ESONE), founded in 1961, also began development of a new
standardized modular system. Along with these systems, numerous commercial companies began working on
various systems of modular nuclear electronics. Further, the independent U.S. national laboratories began
developing modular nuclear electronics systems for their own purposes. As a result, numerous different
nuclear electronics systems were under development, none of which was compatible with any of the other
systems. Overall, research at nuclear laboratories was seriously limited by the compatibility of instruments,
and researchers were forced to invest in numerous different modular nuclear components.

22.6.1 NIM Standard


To remedy this divergent development of nuclear modules, the U.S. National Bureau of Standards (NBS),20
in a 1963 report to the U.S. Atomic Energy Commission (AEC), recommended that the U.S. national
laboratories develop a modular system to be duplicated by commercial manufacturers. The U.S. AEC
convened a meeting of representatives from several national laboratories on Feb. 26, 1964 to determine if
such standardization was of interest to the laboratories. In agreement, the AEC Committee on Nuclear
Instrument Modules (NIM) was established and composed of members from all AEC national laboratories
and a few other prominent nuclear laboratories.
The first NIM Committee meeting was held on March 17, 1964, with follow-up meetings over several
ensuing months. The committee studied the advantages and shortcomings of the existing modular systems,
and a system similar to the CERN design was eventually developed. The prototype bins were manufactured
by Oak Ridge National Laboratory (ORNL), Lawrence Radiation Laboratory in Berkeley, and Lawrence
Radiation Laboratory in Livermore.21 These early prototypes were studied at later meetings of the NIM
Committee and eventually led to a recommended design. Final details were resolved by the NIM Executive

20 The National Bureau of Standards is now the National Institute of Standards and Technology (NIST).
21 The Lawrence Radiation Laboratory in Berkeley is now the Lawrence-Berkeley National Laboratory and the Lawrence Radi-
ation Laboratory in Livermore is now the Lawrence-Livermore National Laboratory.
Sec. 22.6. Instrumentation Standards 1215

bin connector module connector


rear view rear view

top top
34 16 1 1 16 34
28 10 10 28
35 17 2 2 17 35
29 11 11 29
36 18 3 3 18 36
30 12 12 30
37 19 4 4 19 37
31 13 13 31
20 20
38 21 5 5 21 38

22 22
39 6 6 39
23 23

24 24
40 7 7 40
25 25
32 14 14 32
41 26 8 8 26 41
33 15 15 33
42 27 9 9 27 42
bottom bottom
G G

Figure 22.43. Pinout designations for the connectors of nu-


clear instrument modules and bins. From DOE/ER-0457T.

Committee with representatives from the U.S. NBS, ORNL, Lawrence Radiation Laboratory in Berkeley, and
with later added members from Princeton-Pennsylvania Accelerator and Brookhaven National Laboratory
(BNL). The final specifications were published in July 1964, and later updated versions of the specifications
were published in 1966, 1968, 1969, and 1974. The standard was well received, with the first commercial NIM
components made available by November 1964 (see AEC report TID-20893 [1964]). During 1965, numerous
other NIM instruments became available, and NIM components accounted for over 95% of all modular nuclear
instruments produced in the U.S. in the immediate years following 1967. The NIM standard was again revised
in 1990, to make the standard compatible with existent technology and manufacturing processes, as described
in Department of Energy (DOE) document DOE/ER-0457T, where detailed information on power, signal,
connector, and size dimensions are provided in detail. A few of these specifications are outlined below.
Additional information is provided in ORTEC Technical Note 010308 [2008].

Dimensions
A Nuclear Instrument Module (NIM) conforms to a nominal 8.75 inches (22.23 cm) panel height and a basic
width such that a standard size NIM Bin accommodates 12 single-width NIMs or any combination of single-
and multiple-width NIMs with a total of 12 or less unit widths. A unit width for a single Module is 1.32
inches (3.35 cm).22 The Module design permits vertical air flow past the components in a NIM Bin which
is required to provide an open area (reasonably distributed) of not less than 10% of the total horizontal
projection of the Module. Ventilation holes less than 7/64 inch (2.8 mm) diameter are not considered to
abide by the recommended 10% condition and do not apply. The connector pin assignments are designated
as shown in Fig. 22.43 and listed in Table 22.2.

22 Alimited number of Modules with nominal 5.25-inch panel height have been constructed, along with accompanying NIM Bins
with similar reduced dimensions. They are not very popular.
1216 Nuclear Electronics Chap. 22

NIM Bins mount in standard EIA or EC 19-inch racks and are designed to accommodate the size and
pinout of NIMs. Each standard Bin includes 12 sets of guides and 12 Bin Connectors so as to accommodate
up to 12 single-width Modules or any combination of single-width and/or multiple-width Modules with a
total of 12 or less unit widths.23 NIM Bins provide power to the Modules through bussed Bin Connectors
that mate with the Module Connectors. Ample air flow through Bins and power supplies is essential to
provide adequate cooling for both single Bin and stacked Bin systems. This may necessitate the use of fans,
spacers, deflectors, or similar devices. Power at the standard voltages of ±6.00, ±12.00, and ±24.00 DC as
well as 117 volts AC is provided at the Bin busses, as shown in Fig. 22.43 and Table 22.2. The ±6 volt
option is not available on some NIM bins.

Table 22.2. Pinout designations for NIM components. From DOE/ER-0457T.


Pin Function Pin Fun

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