Handbook of Radioactivity

Analysis
Volume 1: Radiation Physics and Detectors

Fourth Edition

Edited by

Michael F. L'Annunziata

ACADEMIC PRESS

An imprint of Elsevier
Handbook of Radioactivity
Analysis
Volume 2: Radioanalytical Applications

Fourth Edition

Edited by

Michael F. L'Annunziata

ACADEMIC PRESS

An imprint of Elsevier
ELSEVIER
Contents of Volume 1

Contributors XXVII VII. Relativistic properties of nuclear

About the Founding Editor xx ix radiation 50
Foreword xxxi A. Relativity 50
Preface to the fourth edition xxxiii Relativistic
B. length contraction and
Acronyms, Abbreviations, and Symbols xxxv time dilation 51

1. Length contraction in relativity 52

2. Time dilation in relativity 53
1. The atomic nucleus, nuclear
interaction of
C. Relativity in cosmic-ray muon
radiation, and the detection and measurement 54
radiation with matter
D. Relativistic measurements of particle
Michael F. UAnnunziata lifetimes 56

1. Bubble chamber measurements 56

Introduction
2. Measurements in CERN muon
II. Discovery and characterization of the
storage ring 57
atomic nucleus and radioactivity 3
E. Energy and mass in relativity 57
III. Basic units and definitions 17
F. Relativistic mass calculations 58
A. Properties of atomic constituents 17
G. Relativistic particle wavelength
B. Nuclides, isotopes, isobars, isomers,
calculations 58
and isotones 18
VIII. Nuclear decay modes 60
C. Mass and energy 20
IX. Nuclear reactions 61
D. Q value 20
A. Reaction types 61
IV. Naturally occuring radionuclides 22
B. Notation 63
A. Radionuclides of cosmogenic C. Energy of reactions (Q value) 64
origin 22
D. Reaction cross section 65
B. Long-lived radionuclides 22
X. Particulate radiation 67
C. Natural radioactive decay chains 22
A. Alpha decay 67
V. Artificially produced radionuclides 23
1. Alpha decay energy 68
VI Properties of the nucleus 27
2. Alpha decay energy and half-life
A. Nuclear radius and density 27

and
relationship 70
B. Nuclear forces, quarks, gluons, 3. Alpha-particle interactions with
mesons 28
matter 71
C. Binding energy 31
B. Beta decay 76
1. Nuclear fission 33
1. Negatron (/8~) emission 76
2. Nuclear fusion 34
2. Positron (/?+) emission 82
3. Nuclear fusion as an energy 3. Electron capture 86
source 35
4. Branching 0", 0+ and EC decay 90
D. Nuclear models 38
5. Double beta (PP) decay 92
1. Liquid drop model 39
6. Parity violation in beta decay 95
2. Shell model 41
7. Beta-particle interactions with
3. Collective model 44
matter 100
E. Superheavy nuclei 46
8. Beta particle absorption and
F. Cluster radioactivity 49
transmission 104

v
vi Contents of Volume 1

C. Internal conversion electrons 106 C. Sample calculations 182

D. Auger and Coster-Kronig electrons 107 1. Nuclear recoil from alpha

E. Neutron radiation 111 emissions 182

1. Discovery of the neutron 111 2. Nuclear recoil from beta

2. Neutron classification 111 emissions 182

3. Neutron sources 116 3. Nuclear recoil from gamma-ray

4. Interactions of neutrons with photon, X-ray photon, or neutrino
matter 126 emissions 183

5. Neutron attenuation 129 D. Radioactive recoil effects 184

6. Neutron decay 134 1. Szilard—Chalmers process 184

F. Proton and neutron radioactivity 134 2. Radioactive disequilibrium 186

1. Protonradioactivity 135 XIV. Cosmic radiation 186

2. Neutron radioactivity 139 A. Classification and properties 188

G. Neutrino interactions with matter 142 B. Showers of the cosmic radiation 191
XI. Electromagnetic radiation —

photons 146 C. Cosmic-ray muon detection and

A. Dual nature: wave and particle 146 measurement 194

B. Gamma radiation 148 D. Cosmic rays underground 194

C. Annihilation radiation 150 E. Origins of cosmic radiation 196

D. Line-spectra X-radiation and F. Cosmic microwave background
bremsstrahlung 151 radiation 196

1. X-rays characterized by discrete XV. Radiation dose 197

spectral lines 151 XVI. Stopping power and linear energy

2. Bremsstrahlung 153 transfer 200
3. Bremsstrahlung and line spectra A. Stopping power 200

X-rays from beta-particle emitters 158 B. Linear energy transfer 203

E. Cherenkov radiation 159 XVII. Radionuclide decay, ingrowth, and

1. Origin and characteristics 160 equilibrium 205

2. Threshold condition 162 A. Half-life 206

3. Threshold energies 163 B. General decay equations 211

4. Applications 163 C. Secular equilibrium 212

F. Synchrotron radiation 164 D. Transient equilibrium 214

1. Synchrotron radiation from natural E. No equilibrium 216

sources 164 F. More complex decay schemes 217

2. Discovery of synchrotron radiation 164 XVIII. Radioactivity units and radionuclide

3. Synchrotron radiation and mass 218

accelerated electron properties 165 A. Units of radioactivity 218

Synchrotron
4. radiation
production B. Correlation of radioactivity and
and
applications 166 radionuclide mass 218

XII. Interaction of electromagnetic radiation C. Carrier-free radionuclides 219

with matter 169 References 220

A. Photoelectric effect 169 Michael F. L'Annunziata 243

B. Compton effect 169

C. Pair production 171 .
Gas ionization detectors
D. Combined photon interactions 176
Georg Steinhauser and Karl Buchtela
XIII. Radioactive nuclear recoil 180

A. Relativistic expressions 180 I. Introduction: principles of radiation

B. Nonrelativistic expressions 181 detection by gas ionization 245
1. Nuclear recoil energy from II. Characterization of gas ionization

alpha-particle emissions 181 detectors 246

2. Nuclear recoil energy from A. Ion chambers 246

gamma-ray photon, X-ray photon, B. Proportional counters 247

and neutrino emissions 181 C. Geiger—Miiller counters 248
 Contents of Volume 1 vii

III. Definition of operating characteristics of D. Self-quenched streamer 288

gas ionization detectors 248 E. Long-range alpha detectors 289

A. Counting efficiency 248 F. Liquid ionization and proportional

B. Energy resolution 248 detectors 292

C. Resolving time 248 References 292

D. Localization 249 Further reading 304

IV. Ion chambers 249 Prof. Dr. Georg Steinhauser 305

A. Operating modes of ion chambers 249 Prof. Dr. Karl A. Buchtela 305

1. Ion chambers operating in the

current mode 249 3. Solid-state nuclear track detectors
2. Charge integration ionization
Shi-Lun Guo, Bao-Liu Chen and S.A. Durrani
chambers 249
3. Pulse mode ion chambers 250 Part 1: Elements 309
B. Examples and applications of ion I. Introduction 309

chambers 250 II. Detector materials and classification of

1. Calibration of radioactive sources 250 solid-state nuclear track detectors 310

2. Measurement of gases 250 A. Crystalline solids 311

3. Frisch grid ion chambers 251 1. Muscovite mica 311

4. Radiation spectroscopy with ion 2. Apatite 313

chambers 252 3. Zircon 314
5. Electret detectors 253 4. Sphene 314

6. Fission chambers 254 5. Olivine 314

V. Proportional gas ionization detectors 255 6. Pyroxene 315
A. Examples and applications of 7. Whitlockite 315

proportional counters 256 8. Other crystalline solids 316

1. Gross alpha—beta counting, B. Glasses 316

alpha—beta discrimination, and 1. Man-made glasses 316

radiation spectroscopy using 2. Natural glasses 317

proportional gas ionization counters 256 C. Plastics 318

2. Position-sensitive proportional 1. CR-39 (polyallyldiglycol carbonate,
counters 258 PADC, PM-355, PM-500, PM-600) 318
3. Low-level counting techniques using 2. Polycarbonate (PC, Lexan, Makrofol,
proportional gas ionization Taffak) 319
detectors 268 3. Cellulose nitrate (CN, LR-115,
4. Application in environmental Daicell) 321

monitoring and health physics 270 4. Polyethylene terephthalate (PET,

VI. Geiger—Muller counters 276 Mylar, Cronar, Melinex, Lavsan,
A. Designs and properties of Geiger—Muller Terphane, Hostphan) 322
counters 276 5. CR-39—DAP series 322
1. Fill gas 276 6. Polyimide (PI, Kapton, Upilex) 323
2. Quenching 276 7. Other new track detector materials 324
3. Plateau 277 III. Recordable particles with solid state
4.Applications 277 nuclear track detectors 325
VII. Special types of ionization detectors 279 A. Protons 325
A. Neutron detectors 279 1. Suitable detectors for proton
1. BF3 tube construction 282 detection 325
2. Fast neutron detectors 282 2. Proton intensity measurements 326
3. Neutron counting in nuclear analysis 3. Proton energy measurements 326
of fissile materials and radioactive 4. Obtaining mono-energetic proton
waste 285 beam for track detector calibration 327
4. Moisture measurements 286 5. Proton spatial distribution
B. Multiple sample reading systems 287 measurements 328
C. Self-powered detectors 288 6. Applications of proton detection 328
viii Contents of Volume 1

B. Alpha particles 329 B. Track formation mechanisms 350

1. Suitable detectors for alpha-particle 1. Ion explosion spike for inorganic
detection 329 solids 350
2. Alpha-particle intensity 2. Chain breaking mechanism in high
measurements 329 polymers 351

3. a-particle energy measurements 331 C. Criteria of track formation 351

4. a-particle spatial distribution 1. Primary ionization rate criterion 351

measurements 332 2. Restricted energy loss for plastic

5. Applications of a-particle detection 332 track detectors 352
C. Fission fragments 333 3. Energy deposition model (ev) 352
1. Suitable detectors for fission D. Extended and transitional criterions 353

fragments 333 1. Zgff/iS 353

2. Fission rate determination 336 2.dE/dx transitional parameter 354

3. Determination of detection E. Incapability of the former adopted

efficiency of fission fragments 337 criteria 354

4. Statistical counting method for 1. Incapability to estimate the
determination of detection threshold values of existing track
efficiency 337 detectors 354
5. Critical angle method 339 2. Incapability to design a new

6. Twin fragment method for determi¬ material possessing the expected

nation of detection efficiency 339 threshold value 354
7. Projected track-length method for F. Conflict between track formation
determination of detection criteria and chain breaking mechanism 355

efficiency 343 G. Latent track structures 355

8. Backscattering effect of fission frag¬ 1. IR absorption spectrometery for
ments from substrate and fission polymer track detectors 355

source 345 2. Cross-section of bond breaking by

9. Spatial distribution of fission and heavy ions 355

angular distribution of fission 3. Effective track core radius 356

fragments 345 4. Layered structure of latent tracks 357

10. Application of fission detection 345 5. Chemical etching and OH groups
D. Heavy ions (Z > 3) 346 in polymers 357
1. Suitable detectors for heavy ions Z 6. Radial Electron Fluence around ion
> 3 346 tracks 358
2. Identification of charge Z 346 V. Track revelation 359
3. Identification of mass A of isotopes 346 A. Chemical etching 359
4. Heavy-ion energy determination 346 1. Etching condition 359
5. Applications of heavy-ion detection 346 2. Track etching geometry 360
E. Neutrons 347 3. Critical angle of etching 360
1. Principles of neutron detection 347 4. Techniques of critical angle
2. Suitable detectors for neutron measurements 360
detection 347 5. Track
etching geometry 361
3. Neutron intensity measurements 348 6. Progress in track etching geometry 361
4. Neutron energy measurements 348 B. Electrochemical etching 362
5. Neutron dosimetry 348 C. Track etching kinetics 362
6. Applications of neutron detection 349 1. Objectives and required parameters 362
F. Exotic particle detection 349 2. Forward calculation 363
1. Suitable detectors for exotic particle 3. Inverse calculation 364
detection 349 VI. Particle identification 364
2. Magnetic monopole detection 349 A. Maximum track length method 364
3. Dark matter particle detection 350 B. Track etch rate versus radiation damage
IV. Track formation mechanisms and density method 364
criterions 350 C. Track etch rate versus residual range
A. Introduction 350 method 364
 Contents of Volume 1 ix

D. Track diameter method for identification 4. Continental drift and ocean-bottom

of charge Z at high and relativistic speading 385

energy 365 5. Archeology and anthropology 385

E. Track length method for identification 6. Tectonic up-Lift rate determination 386
of charge Z at high and relativistic B. Geothermal chronology 387

energy 367 C. Uranium and oil exploration and

VII. Track fading and annealing 367 earthquake prediction 388
A. Track fading and
annealing 368 IV. Life and environmental sciences 389
B. Mechanisms of track fading 368 A. Radiation protection dosimetry 389
C. Arrhenius diagram 368 1. Radon and thoron monitoring and
D. Application of track fading and dosimetry 389

annealing 368 2. Neutron dosimetry 389

1. Problems resulting from track fading 368 B. Environmental sciences 390
2. Improving analysis with the aid of 1. Radioactive fallout from nuclear
track annealing 369 accidents 390
3. Apparent fission track age and its 2. Drainage contamination of nuclear
corrections 369 plants 391
4. Geothermal chronology 369 V. Nanotechnology and radiation induced
VIII. Instrumentation 369 material modifications 391
A. Size of latent tracks and etched tracks 369 Acknowledgments 392
B. Optical microscope 370 References 392
C. Track image analyser Further
370 reading 406
D. Electron microscope 370 Shi-Lun Guo 407
E. Scanning tunneling microscope (STM) Bao-Liu Chen 407
and atomic force microscope 370
F. Spark counter 371 4. Semiconductor detectors
Part 2: Applications 371
Ramkumar Venkataraman
I. Introduction 371
II. Physical sciences and nuclear technology 371 1. Introduction 410
A. Cluster radioactivities A. The
371 gas-filled ionization chamber 410
B. Heavy ion interactions 372 B. The semiconductor detector 410
1. Relativistic projectile fragmentation 372 C. Fundamental differences between Ge
2. Sequential fission after inelastic and Si detectors 412
collisions 372 1. The energy gap 412
C. Nuclear fission and neutron physics 372 2. The atomic number 412
1. Nuclear fission 372 3. The of the
purity or resistivity
2. Neutron physics 374 semiconductor material 413
D. Plasma physics 374 4. Charge carrier lifetime i 414
1. Laser acceleration 374 II. Ge detectors 414
2. Inertial confinement fusion 375 A. High-purity Ge detectors: merits and
E. Astrophysics and cosmic rays 375 limitations 414
F. Nuclear technology 376 B. Analysis of typical y spectra 414
1. Nuclear reactor physics 376 of
1. Spectrum a source emitting a
2. Accelerator-driven subcritical single y ray with Ey < 1022 keV 416
reactors 377 2. Spectrum of a multiple-y-ray source
3. Nuclear forensic
analysis and emitting at least one y ray with an
nuclear
safeguards 377
energy >1022 keV 418
G. Elemental analysis and mapping 380 3. Peak summation 419
III. Earth and planetary sciences 381 4. True coincidence summing effects 419
A. Fission track dating 381 5. Ge-escape peaks 423
1. Absolute approach 381 C. Standard characteristics of Ge detectors 423
2. Zeta approach 383 1. Energy resolution 423
3. LA-ICP-MS-based fission track dating 384 The
2. peak-to-compton ratio 427
3. The detector efficiency 427
x Contents of Volume 1

D. Background and background reduction 431 References 486

1. Background in the presence of a Further reading 490

source 431 Ramkumar ("Ram") Venkataraman 491

2. Background in the absence of the

source 432 5. Alpha spectrometry
3. Background of cosmic origin 432
Nora Vajda, Roy Pollanen, Paul Martin and
4. Background reduction 443

E. The choice of a detector 445

Chang-Kyu Kim
1. General criteria 445 I. Introduction 494

2. Increasing the size of high-purity II. Alpha decay and alpha particle—emitting
germanium detectors 445 radionuclides 495

3. The germanium well-type detector 446 III. Detection systems 500

4. Limitations to the "relative efficiency" A. Detectors 501

quoted for coaxial detectors 446 1. Interaction of alpha radiation with

5. The Broad-Energy Germanium, or detector materials 501

"BEGe" detector 447 2. Characterization of spectroscopic

ill. Si detectors 448 detectors 502

A. Si(Li) X-ray detectors 448 3. Gas ionization detectors 503

B. Si-charged particle detectors 448 4. Semiconductor silicon detectors 505

1. Alpha detectors 449 5. Scintillation detectors 507

2. The Si drift detector technology 453 6. Cryogenic detectors 510

3. Electron spectroscopy and P counting 453 B. Electronic units 511

4. Readout of scintillators 454 IV. Characteristics of the alpha spectrum 512

5. Continuous air monitoring 455 A. Peak shape and spectrum analysis 512

IV. Cadmium zinc telluride detectors 458 1. Peak shape and spectrum analysis
A. Characteristics of cadmium zinc telluride with Si detectors 512
detectors 458 2. Peak shape and spectrum analysis
B. Crystal growth techniques 458 with gas ionization detectors 520
1. The Bridgman process 458 3. Peak shape and spectrum analysis
2. Traveling heater method 459 with liquid scintillation detectors 520

C. Correction schemes to mitigate

poor 4. Peak shape with cryogenic
hole mobility in cadmium zinc telluride detectors 521
detectors 459 B. Counting efficiency 522
1. Frisch
grid device
configuration 460 C. Background and contamination in alpha
Coplanar grid device configuration
2. 460 spectrometry 523
V. Spectroscopic analyses with D. Stability of the alpha spectrometer 523
semiconductor detectors 460 V. In situ alpha spectrometry with Si
A. Sample preparation 462 detectors 525
1. Sample preparation for alpha A. Sampling and simplified sample
spectrometry 462 processing 525
2. Sample preparation for gamma B. Data acquisition 526

spectrometry 470 C. Spectrum analysis tools 528

B. Analysis—analytical considerations 471 D. Alpha spectrometry combined with
1. Analytical considerations in alpha other analysis techniques 529

spectrometry 471 VI. Radiochemical processing 529

2. Analytical considerations in gamma A. Sample preparation and pretreatment 534

spectrometry 472 1. Preparation of solid samples 534

VI. Advances in HPGe detector technology: 2. Preconcentration of liquid samples

gamma-ray imaging with HPGe detectors 481 and sample solutions 535
VII. Segmented Ge detectors and their B. Chemical separation 536
applications in nuclear physics research 482 1. Separations by liquid—liquid
A. Segmented HPGe detectors 483 extraction 536
B. Neutrinoless double beta decay 483 2. Separations by 540
ion exchange
C. Majorana collaboration 484 3. Separations by extraction
D. GERDA collaboration 484 chromatography 544
 Contents of Volume 1 xi

C. Alpha source preparation 551 C. External standard quench indicating

VII. Determination of activity and recovery 553 parameters 595

A. Calibration 553 1. External standard (source) channels

B. Measurement procedure 554 ratio (ESCR) 596

C. Alpha spectrum evaluation 554 2. H-number (H#) 597

1. Principle of evaluation 554 3. Relative pulse height (RPH) and

2. Nuclide identification 554 external standard pulse (ESP) 599

3. Peak area determination for 4. Spectral quench parameter of the

nonoverlapping peaks 555 external standard or SQP(E) 600

4. Peak area determination with 5. Transformed spectral index of the

correction for overlapping peaks 555 external standard (tSlE) 601

5. Calculation of results 556 6. G-number (G#) 604

6. Calculation of the combined D. Preparation and use of quenched

standard uncertainty 556 standards and quench correction
7. Calculation of the decision curves 606

threshold and the detection 1. Preparation of

quenched standards 606
limit 559 2. Preparation of a quench correction
VIII. Quality control 559 curve 608

A. Quality control foralpha spectrometers 559 3. Use of a quench correction curve 609
B. Validation of the procedure 559 E. Combined chemical and color quench
IX. Conclusions 560 correction 609
Terms and definitions, symbols, and F. Direct DPM methods 611
abbreviations 561 1. Conventional integral counting
References 561 method (CICM) 611
Dr. Nora Vajda 572 2. Modified integral counting method
Dr. Roy Pollanen 572 (MICM) 612
Paul Martin 573 3. Efficiency tracing (ET) with 14C 613

Chang-Kyu Kim 573 4. Multivariate calibration 617

VI. Analysis of X-ray, gamma-ray, atomic
6. Liquid scintillation analysis: principles electron, and positron emitters 618

and practice VII. Common interferences in liquid

scintillation counting 623
Michael F. L'Annunziata, Alex Tarancon, Hector
A. Background 623
Bagan and Jose F. Garcia
B. Quench 624

I. Introduction 576 C. Radionuclide mixtures 624

II. Basic theory 577 D. Luminescence 625

A. Scintillation process 577 1. Bioluminescence 625

B. Alpha-, beta-, and gamma-ray 2. Photoluminescence and
interactions in the LSC 579 chemiluminescence 625
C. Cherenkov photon counting 581 3. Luminescence control,
III. Liquid scintillation counter (LSC) or compensation, and elimination 626

analyzer (LSA) 581 E. Static 628

IV. Quench in liquid scintillation counting 584 F. Wall effect 629
V. Methods of quench correction in liquid VIII. Multiple radionuclide
analysis 630
scintillation counting 588 A. Conventional dual- and triple-radio-
A. Internal standard (IS) method 588 nuclide analysis 630
B. Sample spectrum characterization 1. Exclusion method 630
methods 589 2. Inclusion method 631
1. Sample channels ratio (SCR) 589 B. Three-over-two fitting and digital
2. Combined internal standard and overlay technique (DOT) 641

sample channels ratio (IS-SCR) 590 C. Full spectrum DPM (FS-DPM) 641
3. Sample spectrum quench D. Recommendations for multiple

indicating parameters 591 radionuclide analysis 644

xii Contents of Volume 1

E. Complex spectral analysis 644 2. Simplified digital charge-

1. Most-probable-value theory 645 comparison (SDCC) method 703

2. Spectral fitting, unfolding, and 3. Pulse gradient analysis (PGA) 704

interpolation 648 4. Zero-crossing method 705

3. Spectral fitting and subtraction 651 5. Time-of-flight (TOF) spectrometry 706

4. Modeling from spectral library 654 6. General research into n/y

5. Spectral unfolding by region count discrimination 709

ratios 655 XI. Double beta ((8/5) decay detection and

6. Multivariate calibration 657 measurement 709

Radionuclide standardization via LSA 658 A. KamLAND-Zen project 711

A. CIEMAT/NIST efficiency tracing 658 B. SNO+ project 713

1. Theory and principles (3H as the C. EXO-200 project 714

tracer) 659 D. ZICOS project 715

2. Procedure 662 XII. Detection and measurement of

3. Specific examples 663 neutrinos 716

4. Sample, cocktail, and A. Reines and Cowan reaction 716

spectrometer stability 668 B. Liquid scintillation schemes for

5. Cross-efficiency curves 671 neutrino detection and measurement 717

6. 54Mn as tracer nuclide 675 1. Neutrino-electron scattering 717

7. Ionization quenching and 2. Reines-Cowan inverse beta decay

efficiency calculations (3H or reaction 718

54Mn as the tracer) 675 3. Inverse beta decay (charged current

8. Other factors affecting efficiency interactions) yielding negatrons and

calculations 676 unstable nuclei 719

9. Radionuclides in decay chains 677 4. Neutrino charged current

10. Electron capture radionuclides 678 interactions with 13C 720

11. Applications with plastic C. Collaborations for LS neutrino

scintillation microspheres 680 detection and measurement 720

12. Radionuclide mixtures 680 XIII. Microplate liquid scintillation counting 721

B. Secondary standardization by the A. Detector design and background

cross-efficiency method 680 reduction 721

C. Triple-to-double coincidence ratio B. Applications 722

(TDCR) efficiency calculation C. Advantages and disadvantages 722

technique 682 XIV. PERALS, LS alpha-spectrometry with

1. Principles 682 LAAPDs, and MNPs 723

2. Free-parameter model 686 A. PERALS spectrometry 723

3. Experimental conditions and B. Extractive scintillators and solvents for

efficiency calculations 686 Alpha LS spectrometry 724

4. The TDCR efficiency calculation C. Extractive magnetic nanoparticles

technique in a nutshell 688 (MNPs) forAlpha LS spectrometry 725

5. Commercially available 3PM liquid D. Applications of PERALS spectrometry 726

scintillation analyzers 689 E. LS alpha-spectrometry with LAAPDs 728

6. Additional TDCR developments 691 XV. Simultaneous a//? analysis 729

D. Compton Efficiency Tracing (CET) A. Detectors 730
method 693 B. Establishing the optimum PDD setting 731
E. 47rfi-y coincidence counting 694 1. Equivalent a and (3 spillover
Neutron/gamma-ray measurement and criteria 731
discrimination 694 2. Inflection point criteria 732
A. Detector characteristics and properties 694 3. Plateau criteria 732
B. Neutron/gamma-ray (n/y) C. a//? spillover corrections and activity
discrimination 701 calculations 735
1. Digital charge-comparison (CC) D. Optimizing a/(3 discrimination in PDA 735
method 701 E. Quenching effects in a//?
discrimination 737
 Contents of Volume 1 xiii

F. Practical applications of a/p IV. Solubilization 813

discrimination and analysis 738 A. Systems 813
XVI. Plastic scintillators in LSC 741 B. Sample preparation methods 815
XVII. Scintillation in noble liquids 748 1. Whole tissue 815
XVIII. Radionuclide identification 750 2. Muscle (50—200 mg) 815
XIX. AIR luminescence counting 753 3. Liver 815
XX. Liquid scintillation counter performance 755 4. Kidney, heart, sinew, brains, and
A. Instrument normalization and stomach tissue 818
calibration 755 5. Feces 818
B. Assessing LSA performance 756 6. Blood 819
1. New commercial counters 756 7. Plant material 819
2. New custom-made counters 758 8. Electrophoresis gels 821
3. Routine instrument performance V. Combustion 822
assessment 760 VI. Comparison of sample oxidation and
C. Optimizing LSC performance 763 solubilization techniques 822
1. Counting region optimization 763 A. Solubilization 823
2. Vial size and type 764 B. What is sample combustion? 824
3. Cocktail choice 766 C. Advantages and disadvantages 824
4. Counting time 766 1. Solubilization methods and
5. Background reduction 767 suitability 825
6. Conclusions 769 2. Sample combustion methods and
References 769 suitability 825
Further reading 798 VII. Carbon dioxide and
trapping counting 827
Michael F. LAnnunziata 800 A. Sodium hydroxide 827
Alex Tarancon 800 B. Hyaminehydroxide 827
Hector Bagan 801 C. Ethanolamine 828
Jose F. Garcfa 801 D. CarbonTrap and Carbo-Sorb E 828
VIII. Biological samples encountered in
Sample preparation techniques for absorption, distribution, metabolism, and

liquid scintillation analysis excretion 830

A. Urine 830
James Thomson and Simon Temple
1. Sample preparation 830
I. Introduction 804 B. Whole blood 831
II. Liquid scintillation counting cocktail 1. Sample preparation 831

components 804 C. Plasma and serum 833

A. Solvents 804 1. Sample preparation 833
B. Scintillators 805 D. Muscle, skin, heart, brains, and
C. Surfactants 806 stomach 833
1. Nonionics 806 1. Sample preparation 834
2. Anionics 807 E. Liver and kidney 834
3. Cationics 807 1. Sample preparation 834
4. Amphoterics 807 F. Fatty tissue 835
D. Cocktails 808 1. Sample preparation 835
III. Dissolution 808 G. Feces 836
A. Anions 808 1. Sample preparation 836
B. Low ionic strength buffers 808 H. Homogenates 836
C. Medium-ionic-strength buffers 811 I. Solubilization and combustion 836
D. High-ionic-strength buffers 811 IX. Filter and membrane counting 837
E. Acids 811 A. Elution situations 838
F. Alkalis 812 B. Sample collection and filters 838
G. Other aqueous sample types 812 C. Filter and membrane types 839
H. Selection and suitability of a cocktail D. Sample preparation methods 839
based on ionic strength 813 1. No elution 839
2. Partial elution 839
xiv Contents of Volume 1

3. Complete elution 840 IV. Glow discharge mass spectrometry 868

X. Sample stability troubleshooting 840 A. Principle of ionization in a glow
A. Decreasing count rate 840 discharge 868
B. Increasing count rate 841 B. Applications 868
C. Reduced counting efficiency 841 1. Trace and bulk analysis of nuclear
XI. Swipe assays 841 samples 868
A. Wipe media and cocktails 841 2. Determination of radioisotopes in
B. Regulatory considerations 842 the environment 869
C. Practical considerations 842 3. Determination of
isotopic
D. General procedure for
wipe testing 842 compositions 869
XII. Preparation and use of quench curves in 4. Depth profiling measurements 869

liquid scintillation counting 843 V. Secondary ion mass spectrometry 869

A. Chemical quench 843 A. Principle of ionization through ion
B. Color quench 843 impact 869
C. Measurement of quench 843 B. Applications 871
D. Quench curve 844 1. Radioecology 871
1. Preparation of quench curves 844 2. Safeguards and nonproliferation
2. Notes on using the quench curves 846 control 871
3. Color quench 846 3. Cosmochemistry 872
4. Quench curve errors 846 4. Geosciences 872
5. Using a quench curve 848 5. Trace analysis 872
E. Quench correction using selectable 6. Radiochemistry and material
multichannel
analyzer 848 sciences 872
XIII. Environmental sample preparation 849 VI. Inductively coupled plasma mass

A. Extraction chromatographic sample spectrometry 872

preparation 850 A. Principle and instrumentation 872

B. Aqueous sample preparation 851 B. Sample introduction 874
XIV. Waste cocktails—environmental 1. Nebulization 874

consequences 853 2. Hyphenated systems 875

A. Generation of waste cocktails 853 3. Laser ablation 875
B. Disposal methods 853 C. Applications to radionuclides 875
C. Biodegradability 853 1. Methodical developments on isotope
1. Testing for biodegradability 856 ratios 875

2. Biodegradability test methods 856 2. Radioecology 876

D. Incineration 857 3. Treatment and storage of nuclear

E. Legislation and regulatory information 857 waste 876
F. Waste cocktails—the way forward 858 4. Application to Chernobyl and
Acknowledgments 859 Fukushima samples 877
References 859 VII. Resonance ionization mass spectrometry 878

Further reading 860 A. Principle and requirements for the laser

light sources 878

Radioisotope mass spectrometry B. Resonance ionization mass

spectrometry systems and applications 880

Clemens Walther and Klaus Wendt
1. Elemental-selective resonance

I. Introduction 861 ionization mass spectrometry using

II. Figures of merit 864 pulsed lasers 880
III. Thermal ionization mass spectrometry 866 2. Highest isotopic selectivity using
A. Principle of surface ionization 866 continuous wave lasers 882
B. Applications 867 VIII. Accelerator mass spectrometry 883
1. Isotope ratio determination with A. Principle 883
thermal ionization mass B. Applications of accelerator mass

spectrometry 867 spectrometry 886

2. High-sensitivity measurements with 1. Radioisotope dating in archeology
thermal ionization mass and other applications of the isotope
spectrometry 867 14C 886
 Contents of Volume 1 xv

2. Accelerator mass spectrometry V. Automated solid scintillation analyzers 943

applications in geo- and A. Automated gamma analysis 943

cosmoscience 886 1. Multiple detector design 943
3. Noble gas analysis 886 2. Multiuser automatic gamma activity
4. Accelerator mass spectrometry analysis 946
in life sciences 887 3. Multiple gamma-emitting nuclide
5. Accelerator mass spectrometry analysis 946
measurements on long-lived B. Microplate scintillation analysis 951
radionuclides in the environment 887 1. Solid scintillation counting in
References 888 microplates 951
Clemens Walther 898 2. Scintillation proximity assay 955
Klaus D.A. Wendt 898 VI. Detection of neutrons 962
A. Inorganic neutron scintillators 963
9. Solid scintillation analysis B. Solid organic neutron scintillators 968
C. Neutron detectors with scintillating and
Michael F. L'Annunziata
optical fibers 972
I. Introduction 900 1. Scintillating fibers arrays 972
II. Principles of solid scintillation 901 2. Optical fiber—neutron detector
A. Inorganic crystal scintillators and their arrays 975

properties 901 VII. Scintillation in plastic media 978

B. Scintillation mechanisms in inorganic A. The scintillation process in plastic 978

crystals 905 B. Applications of

plastic scintillators 980
C. Conversion of detector scintillations to VIII. n/y pulse shape discrimination 980

voltage pulses 908 IX. Bonner sphere neutron spectrometry 983

III. Solid scintillation analyzer 909 X. Lucas cell 987
A. Scintillation crystal detectors 909 XI. PHOSWICH detectors 989
1. Planar detector 910 A. Simultaneous counting of a-, /?-,
2. Well-detector 910 and y-rays or a-, /?(y)-rays, and
3. Through-hole detector 912 neutrons 989
B. Photomultipliers 913 B. Remote glass-fiber-coupled phoswiches 991
1. Dynode photomultiplier or PMT 913 C. Low-level counters 992
2. Hybrid photomultiplier tube 914 D. Simultaneous of fields
counting n/y/p 992
3. MicroChannel plate photomultiplier 915 E. Neutron spectrometry 995
4. Channel photomultiplier 917 F. Simultaneous beta- and gamma
5. Semiconductor photomultipliers 918 spectroscopy 996
C. Pulse height discriminators 928 G. Other phoswich detectors 999
D. Single-channel analyzer 928 H. Analytical expressions 1000
E. Multichannel analyzer 929 XII. Neutrino interactions 1001
F. Other components 932 XIII. Double beta ((3(3) decay measurements 1002
IV. Concepts and principles of solid XIV. Scintillating bolometers 1008
scintillation analysis 932 A. Operating principle 1008
A. Gamma-ray spectra 932 B. Search for neutrinoless double beta
B. Counting and detector efficiencies 933 (Ov(3(3) decay 1010
1. Counting efficiency 933 C. Search for weakly interacting massive
2. Detector efficiency 934 particles 1013
C. Sum-peak activity determinations 936 References 1014
D. Modified sum-peak activity Further reading 1044
determinations 939 Michael F. L'Annunziata 1045
E. Self-absorption 940
F. Counting geometry 941 Index 1047
G. Resolution 941
H. Background 942
Contents of Volume 2

Contributors B. Dose monitoring

About the Founding Editor VI. Mobile monitoring
Foreword A. Aerial measurements
Preface to the fourth edition B. Mobile laboratories

Acronyms, Abbreviations, and Symbols References

Further reading
1. Environmental radioactivity Rudolf Engelbrecht
monitoring
2. Environmental liquid scintillation
Rudolf Engelbrecht
analysis
I. Introduction:objective of environmental
Xiaolin Hou and Xiongxin Dai
monitoring
II. Types of monitoring programs I. Introduction
A. Routine monitoring II. Low-level liquid scintillation counting
B. Emergency preparedness theory
C. Emergency monitoring A. Sources of background
III. Fundamentals of environmental monitoring B. Background reduction methods—
A. Design of environmental monitoring instrument considerations

programs 1. Enhanced passive/graded shielding

B. Sampling strategies 2. Active guard detectors
C. Sample preparation 3. Pulse discrimination electronics
D. Measurement and quantification 4. TR-LSCquasi-active detector guards
E. Quality assurance/quality control 5. Counting region optimization
IV. Monitoring for internal exposure 6. Process optimization
A. Air C. Background reduction methods—vial,
1. Aerosols vial holder, and cocktail considerations
2. Online offline systems
versus 1. Vials
3. Gaseous effluents 2. Vial holders
B. Soil, sediments, vegetation, and deposits 3. Cocktail choice and optimization
1. Laboratory based D. Background reduction
2. In situ gamma spectroscopy methods—environment
C. Water III. Alpha/beta discrimination
1. Wastewater A. Alpha/beta separation theory
2. Rain B. Alpha/beta instrumentation
3. Groundwater 1. The PERALS spectrometer
4. Surface water 2. Conventional LS spectrometers with
5. Drinking water pulse-shape discrimination
D. Foodstuff C. Cocktail and vial considerations
1. Milk 1. Cocktail choice
2. Meat and fish 2. Vial choice
3. Vegetables, fruits, and cereals D. Alpha/beta calibration
4. Mixed diet 1. Misclassification Calculations
V. Monitoring for external exposure 2. Quenching and correction of
quench
A. Dose rate monitoring percentage misclassification

xvi
 Contents of Volume 2 xvii

IV. Triple-to-double coincidence ratio D. Radium

(TDCR) counting 1. Environmental occurrence and
A. TDCR liquid scintillation counting importance
B. TDCR Cerenkov counting 2. Sample preparation and
V. Analysis of alpha-emitting transuranic measurement of 226Ra, 228Ra,
nuclides 224Ra, and 223Ra
A. Environmental occurrence and E. Lead-210 (210Pb) [Bismuth-210 (210Bi)
importance and Polonium-210 (210Po)]
B. Sample preparation and analysis 1. Environmental occurrence and
1. Alpha spectrometry importance
2. Mass spectrometry Sample preparation and
2. analysis
3.Liquid scintillation counting (LSC) F. Thorium
VI. Analysis of beta-emitting radionuclides 1. Environmental occurrence and
A. Tritium (3H)
importance
1. Environmental occurrence 2. Sample preparation and analysis
2. Sample preparation and analysis VIII. Spectrum deconvolution methods in
B. Radiocarbon (14C) environmental analysis
1. Environmental occurrence A. Spectrum deconvolution, unfolding,
2. Sample preparation and analysis stripping, peak fitting
3. Analysis of 14C in fuels containing B. Approaches in LS beta spectrometry
biogenic materials C. Alpha spectrum unfolding
C. lron-55 (55Fe) 1. Energy resolution
1. Environmental occurrence 2. High energy tailing
2. Sample preparation and analysis 3. Software
D. Nickel-63 (63Ni) D. Better energy resolution enables more

1. Environmental occurrence complete separation

2. Sample preparation and analysis 1. Cocktail and sample quench
E. Strontium-89 and strontium-90/ 2. Vial selection
yttrium-90 (89Sr and 90Sr/90Y) 3. Lower sample temperature
1. Environmental New detector
occurrence 4. designs
2. Sample preparation References
3. LSC measurements Xiaolin Hou
F. Technetium-99 (99Tc) Xiongxin Dai
1. Environmental occurrence

2. Sample preparation and analysis 3. Analysisof environmental

G. Plutonium-241 (241Pu) radionuclides
1. Environmental occurrence
Miroslav Jeskovsky, Jakub Kaizer, Ivan Kontul',
2. Sample preparation and
analysis
H. Other radionuclides (36CI, 41Ca, 129l) Calina Lujaniene, Monika Mullerova and

1. Chloride-36 (36CI) Pavel P. Povinec

2. lodine-129 (129l) I. Introduction

3. Calcium-41 (41Ca)
II. Environmental radionuclides
VII. Analysis of radionuclides from natural A. Primordial radionuclides
decay series B. Radiogenic radionuclides
A. Uranium
C. Cosmogenic radionuclides
1. Environmental occurrence and D. Anthropogenic radionuclides
importance 1. Nuclear weapons testing
2. Sample preparation and analysis 2. Nuclear reactors
B. Gross alpha and beta measurements
3. Nuclear fuel reprocessing plants
C. Radon
4. Nuclear accidents
1. Environmental occurrence and 5. Specific anthropogenic
importance radionuclides
2. Sample preparation and analysis III. Radionuclide compartments
xviii Contents of Volume 2

A. Atmosphere 3. Extraction chromatography

B. Hydrosphere 4. Multistage extraction chromatography
C. Biosphere column methods
D. Pedosphere 5. Combined procedures for the
IV. Analytical techniques determination of neptunium and
A. Radiometric techniques other actinides
1. Alpha spectrometry 6. Source preparation
2. Beta counting 7. Examples of actinides in the
3. Gamma spectrometry environment
B. Low-energy inorganic mass spectrometry VI. International networks for monitoring of
1. Inductively coupled plasma mass environmental radionuclides

spectrometry A. International monitoring system of

2. Thermal ionization mass CTBTO

spectrometry B. European network "Ring of Five"

3. Resonance ionization mass VII. Conclusions

spectrometry Acknowledgments
4. Glow discharge mass spectrometry References
5. Secondary ion mass spectrometry Miroslav Jeskovsky
6. 3H-3He ingrowth mass spectrometry Jakub Kaizer
7. Positive-ion mass spectrometry Ivan Kontul'
C. Accelerator mass spectrometry Galina Lujaniene
1. Ion separation in accelerator mass Monika Mullerova

spectrometry Pavel P. Povinec

2. Ion source

3. Injection system 4. Radioactive aerosol analysis

4. Tandem accelerator
Konstantinos Eleftheriadis and Alexandra
5. High-energy analyzer and ion
loannidou
detection
V. Radionuclide analyses I. Introduction
A. Radioactive gases A. What is a radioactive aerosol?
1. Radiocarbon B. Radioactive aerosol formation
2. Tritium II. Radioactive aerosol and
sampling
3. Argon, krypton, and xenon measurement
4. Radon A. Aerodynamic particle sizing
B. Radionuclides on aerosols 1. Aitken nuclei mode particles
1. Properties of aerosols 2. Accumulation mode particles
2. Sampling of aerosols 3. Coarse-particle mode particles
3. Examples of radionuclides on B. Instrumentation
aerosols 1. High-volume air samplers
C. Radionuclides in freshwater systems 2. Aerosol cascade impactors
1. Sampling of water III. Radioactive aerosols in ambient air
2. Examples of radionuclides in water A. Radon and thoron decay product
systems aerosols
D. Radionuclides in soil B. Radioactive aerosols associated with the
1. Preparation of soil samples for cosmic ray—produced radionuclides
radionuclide analysis C. Radioactive aerosols in the workplace
2. Examples of radionuclides in soil environment
E. Radionuclides in biota 1. Mine aerosols
1. Radiocarbon and tritium D. Radioactive aerosols associated with the
2. Radiocesium and radiostrontium
operation of high-energy particle
3. Radioiodine accelerators
F. Analysis of actinides E. Fission product radionuclide aerosols
1. Sampling and pretreatment 1. Nuclear bomb tests
2. Separation of actinides 2. The comprehensive Test Ban Treaty
 Contents of Volume 2 xix

3. Chernobyl accident C. Polonium-210 and Lead-210

4. Fukushima accident 1. Seawater
IV. Residence time of radioactive aerosols 2. Digestion of filters and sediments
21
A. Residence time of tropospheric aerosol 3. Plating of °Po
particles associated with the cosmic D. Radium isotopes
ray—produced radionuclides 1. Measurement of 223Ra and 224Ra
B. Residence time of tropospheric aerosol 2. Measurement of 228Ra and 226Ra
particles associated with the radon decay E. Radon-222

product radionuclides F. Beryllium-7

C. Residence time of tropospheric aerosol V. Analysis of anthropogenic radionuclides
particles associated with the fission A. Preparation of samples for radionuclide

product radionuclides analysis

References B. Shipboard chemistry for seawater
Further reading samples
Konstantinos Eleftheriadis 1. Transuranics
Alexandra loannidou 2. Cesium
3. Strontium
5. Marine radioactivity analysis C. Laboratory chemistry for seawater

Pavel P. Povinec, Mats

samples
Eriksson, Jan Scholten
1. Transuranics
and Maria Betti
2. Cesium
I. Introduction 3. Strontium
II. Sampling techniques D. Laboratory chemistry for sediment and
A. Seawater sampling biota samples
B. Sediment sampling VI. Activity measurement techniques
C. Biota sampling A. Radiometric methods
D. Sampling of particulate matter 1. Low-level alpha-spectrometry
III. Underwater gamma-ray spectrometry 2. Low-level beta-spectrometry
A. Towed detector systems 3. Low-level gamma-spectrometry
B. Stationary detector systems 4. Underground laboratories
C. Applications of underwater gamma-ray B. Mass spectrometry methods
spectrometry 1. 3He in-growth spectrometry for 3H
1. Mururoa and Fangataufa lagoons analysis
2. Novaya Zemlya bays 2. Inductively coupled plasma mass

3. Mapping of coastal sediments in the spectrometry

Irish Sea 3. Thermal ionization mass

4. Monitoring of 137Cs in Irish spectrometry

Seawaters 4. Resonance ionization mass

5. Submarine groundwater discharge spectrometry

studies 5. Accelerator mass spectrometry
IV. Analysis of natural radionuclides 6. Laser-based 14C spectroscopy
A. Thorium, protactinium, and uranium 7. Positive-ion mass spectrometry
isotopes 8.Comparison of detection limits
1. Sampling of seawater VII. Analysis of radioactive particles
2. Sampling of particulate matter and A. Radioactive particle studies
sediments 1. Safeguards applications
3. Dissolving of particulate matter and 2. Radiological impact studies
sediments 3. Geo-chemical behavior studies of
4. Ion-exchange separation radionuclides
5. Electrodeposition of Th, U, and Pa B. Protocols for studying radioactive
B. Thorium-234 particles
1. Sediments 1. Nondestructive analysis
2. Seawater 2. Semi-destructive analysis of particles
 Contents of Volume 2

3. Destructive analysis on particles D. External standard quench correction

VIII. Management of data quality V. Cherenkov counting parameters
A. Laboratory Information Management A. Sample volume

system B. Counting vials

B. Intercomparison exercises C. Wavelength shifters
C. Reference materials D. Ionic liquids
IX. Marine radioactivity databases E. Refractive index
X. Examples of marine radioactivity studies F.Sample physical state
A. Worldwide marine radioactivity studies VI. Cherenkov counting in the dry state
1. The 137Cs time series in the Atlantic VII. Radionuclide analysis with silica aerogels
Ocean VIII. Cherenkov counting in microplate format
2. The 137Cs time series in the Pacific A. Sample-to-sample cross-talk
Ocean B. Sample volume effects
3. The 137Cs time series in the Indian C. Quench correction
Ocean IX. Multiple radionuclide analysis
4. Radionuclide tracing of water A. Sequential Cherenkov and liquid
masses in the South Indian Ocean scintillation analysis
B. Southern Hemisphere Ocean Tracer 1. Sequential Cherenkov counting and
Studies efficiency tracing
C. Marine radioactivity impact of the 2. 89Sr + 90Sr(90Y) analysis by
Fukushima accident Cherenkov counting with
XI. Conclusions subsequent LSA
Acknowledgments B. Cherenkov analysis with wavelength
References shifters
Pavel P. Povinec X. Radionuclide standardization
Mats Eriksson A. Cherenkov counting efficiency—
Jan Scholten detection probability function,
Maria Betti CHEREN
B. Anisotropy detection model—
Cherenkov counting CHEREN2
C. TDCR Cherenkov counting
Michael F. UAnnunziata, Zeljko Crahek and
Natasa Todorovic
1. Anisotropy detection model
2. Stochastic GEANT4 model in
I. Introduction Cherenkov counting
21
II. Discovery of Cherenkov radiation D. Standardization of °Pb
III. Theory and properties of Cherenkov E. Routine TDCR activity analysis
radiation XI. Gamma ray detection and discrimination
A. Interpretation by ll'ja M. Frank and XII. Particle identification

Igor Y. Tamm A. Threshold and differential Cherenkov

B. Quantum mechanical interpretation counters
C. Threshold condition B. Mirror- or lens-focused RICH counters
D. Threshold energies C. Proximity-focusing RICH counters
E. Photon spatial asymmetry D. Time-of-propagation Cherenkov
F. Photon spectrum and radiation intensity counters
G. Cherenkov photon emissions and E. Time-of-flight Cherenkov counters
counter geometry XIII. Neutrino detection and measurement
IV. Quenching and quench correction A. Large light-water Cherenkov detectors
A. Internal standardization B. Large D2O neutrino target
B. Sample channels ratio C. Neutrino telescopes in lake and ocean

C. Sample spectrum quench indicating floors

parameters D. Neutrino astronomy in Artie ice
1. Counting region E. Radio Cherenkov counting
2. Quench correction XIV. Applications in radionuclide analysis
 Contents of Volume 2 xxi

A. Phosphorus-32 2. Live-timed anticoincidence counting

B. Strontium-89 and Strontium-90 with extending dead-time corrections
(Yttrium-90) 3. Applications of the method of
1. Cherenkov counting of 89Sr with anticoincidence Beta —gamma
90Sr(90Y) Radionuclide standardization
2. Sequential Cherenkov counting and C. Beta—gamma correlations
liquid scintillation analysis 1. Introduction
C. Strontium-90(yttrium-90) exclusive of 2. Theoretical description of the beta-
strontium-89 gamma correlations method
1. Chemical separation and Cherenkov 3. Applications of the Beta —gamma

counting of 90Y correlations method to radionuclide

2. Chemical separation and Cherenkov standardization

counting of 90Sr with 90Y D. Gamma—gamma coincidences

ingrowth 1. Introduction to the sum peak method

D. Yttrium-90 2. Theoretical description of the sum

E. Other applications peak method

XV. Advantages and disadvantages in 3. Dead time and pileup corrections
radionuclide analysis 4. Applications of the
peak sum method
XVI. Recommendations in radionuclide III. Solid angle primary methods
analysis A. 4tc proportional counting
References B. 2tt proportional counting
Further reading C. 47ry counting
Michael F. L'Annunziata D. 4tu windowless sandwich detectors

Zeljko Grahek E. 4ttPy + 4tc sum counting

Natasa Todorovic F. Defined solid angle
G. Internal gas counting
7. Radionuclide standardization 1. Theoretical description of internal gas
counting
Agustm Grau Malonda and Agustih Grau Carles
2. Some experimental aspects of internal
I. Introduction gas counting
II. Absolute direct methods 3. Applications of internal gas counting
A. Beta—gamma coincidences to radionuclide standardization
1. Principles of the method H. Liquid scintillation
counting
2. Radionuclide standardization 1. Importance of the beta spectrum in
methods based on beta—gamma the standardization of Co-60
coincidence I. Calorimetric detectors
3. Applications of the beta—gamma 1. Classiccalorimetry
coincidence method in 2. Cryogenic calorimeter
radionuclide standardization. IV. Relative methods
Differentiationby type of beta counter A. Calibration methods based on gamma
4. Applications of the beta—gamma ray spectrometry
coincidence method. 1. Description of the general method
Standardization of radionuclides and 2. Heath method
determination of nuclear constants 3. Semi-empirical methods
5. Application of the tracer method 4. Monte Carlo technique
6. Applications of a two-dimensional B. Measurement of high activity. Ionization
method of extrapolation chambers
7. Beta-gamma coincidences. 1. Calibration of ionization chamber
Generation of extrapolation curves radionuclides
8. Digital systems for beta-gamma 2. Applications of ionization chambers
coincidence 3. Considerations on the calculation of
B. Beta—gamma anticoincidences ionization chamber efficiency
1. Anticoincidence method with V. Reference systems
nonextending dead time A. The SIR of gammas
xxii Contents of Volume 2

1. Measurement of short half-life VI. Detection limits

A. Critical levels
gamma emitters
B. The SIR of betas B. Gamma Spectra
VI. Preparation of radioactive samples 1. High-resolutiongamma spectra
A. Introduction 2. Low-resolution gamma spectra
B. Sample preparation for radionuclide VII. Metrology applications
metrology A. Uncertainty budget

1. Supports for extended samples B. Uncertainty calculation

2. Dilutions in aqueous solutions 1. Uncertainty transmission in

3. Drops deposit in the sample holder Eq. (8.137)

4. Determination of mass 2. Numerical calculation of
5. Methods for verifying and improving uncertainty
the quality of the source References
References Relevant Statistical References Tables

Agustfn Grau Maionda Agustfn Grau Maionda

Agustfn Grau Carles Agustfn Grau Carles

8. Radioactivity counting statistics 9. High-resolution beta imaging

Agustfn Grau Maionda and Agustfn Grau Carles Nicole Barthe, Serge Maitrejean, Nicolas
Carvou and Ana Cardona (In Memoriam)
I. Introduction
II. Statistical distributions I. Introduction
A. The Poisson distribution II. Autoradiography principles
B. The Gaussian distribution A. History
III. Analysis of a sample of results B. General features
A. Best estimate of the true value 1. Isotopes used
B. Best estimate of precision Physical principles of beta
2.
C. Error propagation interaction and applicability in
D. Accuracy of the mean value high-resolution radionuclide
E. Combination of measurements imaging (autoradiography)
F. Interlaboratory comparisons 3. Sample preparation
1. Philosophy of the Paule and Mandel III. Energy-storage latent imaging
method A. Photographic emulsions
2. Calculation of the variance of the 1. Macroautoradiography with film
between set 2. Microautoradiography with
3. Power-Moderate mean emulsions
4. Power-Moderated weighted Mean B. Phosphor screen technology
(PMM) (autoradioluminography)
G. The statement of the results 1. History
1. Type B calculation of typical 2. General principles
uncertainty 3. Various phosphor screens
2. Combined standard uncertainty 4. Performance
3. Rules for expressing results 5. Quantification methods
IV. Statistical inference Advantages and drawbacks
6.
A. Hypothesis testing Applications
7.
B. Confidence intervals IV. Particle counting imaging systems
C. Statistical inference A. Gaseous detector
1. Variance of a population 1. History: from MWPC to PPAC
2. Variance of two populations (BetalMAGER TRacer) and to
V. Regression micropattern gas detectors
A. Linear regression (BeaQuant)
1. Confidence intervals and hypothesis 2. Description of BetalMAGER TRacer
testing 3. Description of the BeaQuant system
 Contents of Volume 2 xxiii

B. Solid membrane detector (digital 10. Flow-cell radionuclide analysis

microautoradiography) Michael F. LAnnunziata
1. History (BetalMAGER DFine,
formerly Microlmager) I. Introduction
2. Description of the BetalMAGER II. High-performance liquid
DFine chromatography flow-cell analyzers
C. Characteristics and performances of A. High-performance liquid

particle-counting imagers chromatography flow cell analyzers

1. Isotopes used B. Liquid (homogeneous) flow cells
2. Performance C. Solid (heterogeneous) flow cells
3. Quantification D. Gamma and positron emission
D. Data analysis for particle-counting tomography flow cells
imaging systems 1. High-energy gamma cell
1. List mode files 2. Low-energy gamma cell
2. Multiisotope separation according 3. Positron emission tomography cell
to energy E. Narrow-bore and microbore flow cells
3. Multiple isotope separation F. Luminescence flow cell (fLumo)

according to decay G. Hybrid silicon pixel flow cell

V. Comparative use of the different H. Criteria for flow-cell selection

techniques III. Principles of flow scintillation counting

A. Applications in biochemical analysis A. Count rates
B. Advantages and limitations of B. Background and net count rate
radioimagers in histological studies C. Counting efficiency and disintegration
C. Potentialities for multiradionuclide rates

labeling 1. Staticefficiency runs

D. Autoradiography associated with mass 2. Gradient efficiency run
spectroscopy D. Minimal detectable activity
VI. Other applications E. Sensitivity, flow rate, and resolution
A. Biochemistry of development studies F. Precision
B. Bacteriology G. Detection optimization
C. Physiology and gene expression 1. Multichannel analysis
D. Molecular biology 2. Chemiluminescence detection and
E. Molecular imaging correction
F. Nuclear waste decommissioning 3. Time-resolved liquid scintillation
projects (analysis of potential counting
radioactive contamination) H. Instrument performance assessment

VII. Perspectives and future developments IV. Flow scintillator selection

A. Autoradiography to validate in vivo V. Dual-functionality flow-cell detectors
imaging information A. Scintillating extractive resins
1. Preclinical applications. B. Composite bed of scintillating and

Development and validation of extracting particles

new molecular imaging probes bed
C. Equilibrium-based
2. Clinical applications D. Planar mixed-bed flow cell
3. Bremsstrahlung radiation imaging E. Planar detectors based on

4. Cerenkov luminescenceimaging semiconductor diodes

B. Autoradiography and alpha-particle F. Whole-column detector
imaging G. Tritiated water vapor in air detector
VIII. Conclusions VI. Flow-cell radionuclide analysis
References sequential to separation
Further reading A. "Tc in nuclear waste and process
Nicole Barthe monitoring
Serge Martrejean B. Actinides and 90Sr in soil
Nicolas Carvou C. Alpha/beta discrimination
Ana Cardona, in Memoriam
xxiv Contents of Volume 2

D. 89Sr and 90Sr(90Y) analysis IV. Selected radiochemical analysis

E. Cherenkov flow-cell analysis examples
VII. Stopped-flow detection A. Strontium-90
VIII. Flow-cell effluent water monitors B. Technetium-99
A. 3H effluent water monitors C. Actinides
B. Heterogeneous {a—(3) and 7 D. Renewable separation column
discriminating cell applications
IX. Single radionuclide analysis V. Automation using robotics
in high-performance liquid VI. Automated monitors for industrial

chromatography scale nuclear processes

X. Dual radionuclide analysis VII. Radionuclide sensors and systems for
XI. Online HPLC-FSA and mass water monitoring
spectrometry A. Preconcentrating minicolumn sensors
A. HPLC-FSA-MS instrumentation and B. Sensors for "Tc(VII) using quantitative

interfacing capture
B. Representative data C. Equilibration-based radionuclide
XII. Online FSA and nuclear magnetic sensors

resonance D. Sensor probes and systems for water

A. Principle of nuclear magnetic monitoring
resonance spectroscopy VIII. Digital microfluidics for microscale
B. HPLC-FSA-NMR system single bead manipulations
C. HPLC-FSA-NMR representative data IX. Radioisotopes in medicine
XIII. Online HPLC-FSA-MS-NMR A. Therapeutic radionuclides
References 1. Beta emitters
Further reading 2. Alpha emitters
Michael F. L'Annunziata B. Diagnostic radionuclides
1. Gamma emitters
11. Automated radiochemical 2. Positron emitters

separation, analysis, and sensing X. Discussion

Acknowledgments
Jay W. Grate, Matthew J. O'Hara and
References
Oleg B. Egorov
Jay W. Grate, PhD
I. Introduction Matthew J. O'Hara
II. Radiochemical separations Oleg B. Egorov, PhD
A. Separation requirements
B. Radiochemical separation approaches 12. Analytical techniques in nuclear
C. Modern radiochemical separation safeguards
materials
William Geist, Peter Santi and Philip Hypes
III. Automation of radiochemical analysis
using flow injection or sequential I. Introduction
injection fluidics II. Photon-based assay for safeguards
A. Flow injection and sequential A. Introduction: characteristics of U/Pu
injection fluidics and their spectra
B. Sequential injection separations 1. Attribute tests
C. Alternative fluid delivery systems 2. Cerenkov analysis of spent fuel
D. Column configurations 3. Activelength measurements
E. Renewable separation concepts and 4. Sample screening with X-ray
methods fluorescence
F. Lab-on-valve B. Uranium enrichment (infinite thickness)
G. Extractant liquids and particles 1. General approach
H. Detection 2. Correction factors
 Contents of Volume 2 xxv

3. Low-resolution measurements 13. Nuclear forensics

4. High-resolution measurements Michael J. Kristo
5. Specialized geometries (fuel pellets
and rods) I. Introduction

C. Isotopic measurements of uranium and A. What is nuclear forensics?

plutonium II. The origins of nuclear forensics

1. Characteristics of the uranium and A. The policy implications of nuclear
plutonium spectra forensics
2. Ratio-based measurements of B. How the case begins

isotopic composition III. National objectives

3. Typical results from fielded software IV. Nuclear attribution
D. Mass measurements V. Nuclear forensic interpretation
1. Material test reactor fuel VI. Validated signatures
2. efficiency
Customized geometry A. Comparative signatures

modeling B. Predictive signatures

3. Holdup measurements VII. Analytical results

III. Neutron-based assay for safeguards A. Categorization
A. Radiation signatures from plutonium B. Characterization
and uranium C. Full nuclear forensics analysis
B. General neutron counters for VIII. Validated methods

safeguards measurements A. Radioactive material analysis

C. Neutron well counter properties 1. Elemental and isotopic bulk
1. Efficiency analysis tools
2. Die-away time 2. Imaging tools
3. Gate fractions 3. Microanalysis tools
D. Singles neutroncounting B. Traditional forensic analysis
E. Neutron coincidence counting 1. Overview
1. Introduction to coincidence 2. Documentary evidence
counting 3. Impressions
2. Shift register electronics 4. Chemical analysis
3. Passive coincidence counting 5. Tissue and hair evidence
4. Active coincidence counting 6. Weapons evidence
F. Neutron multiplicity counting 7. Tool marks
1. Introduction to multiplicity 8. Fiber examination

counting 9. Flora and fauna

2. Multiplicity shift register electronics 10. Other materials evidence
3. Multiplicity measurements C. Application and sequencing of
IV. Calorimetric assay techniques and methods
A. Introduction IX. Quality assurance
B. Heat flow calorimetry X. Sampling
1. Operating modes for heat-flow XI. Conclusions
calorimeters Acknowledgments
2. Calibrating a heat-flow calorimeter References
3. Types of heat-flow calorimeters Michael J. Kristo
C. Calorimetric assay
1. Assay error determination
2. Calorimetric assay performance
D. Applications Appendix A: Table of radioactive isotopes
References Appendix B: Particle range-energy correlations
William H. Geist Index
Peter Santi

Philip A. Hypes