Radiation Detection Concepts Methods and Devices
Radiation Detection Concepts Methods and Devices
Douglas S. McGregor
J. Kenneth Shultis
First edition published 2020
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Preface xxi
1 Origins 1
1.1 A Brief History of Radiation Discovery 1
1.2 A Brief History of Radiation Detectors 10
vii
viii Contents
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
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
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
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
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.
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
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
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DEARNALEY, G., AND D.C. NORTHROP, Semiconductor Counters
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FLAKUS, F.N., “Detecting and Measuring Radiation—A Short His-
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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
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.
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 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.
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.
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.
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.
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.
2.6 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.
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.
2.8.3 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.
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
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
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.
37
38 Basic Atomic and Nuclear Physics Chap. 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.
• 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)
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
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.
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.
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.
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.
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
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
hν
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
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.
- 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.
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.”
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)
2π
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
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.
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.
∂ 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
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.
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
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
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
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)
nπ
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
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
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
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
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
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
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.
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.
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]
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
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.
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.
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
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.
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.
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.
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
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.,
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
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
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
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.
3.7 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.
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.
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.
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
A ∗
γ decay: ZP →A
ZP + γ . (3.89)
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
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%
α2 (0.0010%) cited states with nuclear masses greater than the ground state
γ ( .00
α3 (0.0065%)
0
γ(
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
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
−
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
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)
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
∗
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.
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.
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
N (t)
P (t) = = e−λt . (3.127)
N (0)
86 Basic Atomic and Nuclear Physics Chap. 3
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)
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.
dN (t) n
= −λ1 N (t) − λ2 N (t) − · · · − λn N (t) = − λi N (t) ≡ −λN (t). (3.133)
dt i=1
n
λ≡ λi . (3.134)
i=1
The probability fi that the nuclide will decay by the ith mode 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
t
N (t) = No e−λt + dt Q(t )e−λ(t−t ) (3.138)
0
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.,
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
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?
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
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).
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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.
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.
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.
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
As x → dx, it is found that P (dx) → μt dx, which is in agreement with the definition of μt .
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.
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.
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
or
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.
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
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,
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,
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.
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 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.
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
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
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
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
T 2A 4A
= (1 − ωc ) = ω2, (4.54)
E (1 + A)2 (1 + A)2 r
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.
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 ]
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.
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
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
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 )
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
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:
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
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.
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].
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].
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 .
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.
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
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
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 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
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),
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
Transformations between the two systems make use of Eqs. (4.47) and (4.48) as well as the interrelationship
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− .
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
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,
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.
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.
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).
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]
Janni [1982] gives the following formula, valid within 10% for Z > 34:
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
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
(−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
- -
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.
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
#
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
[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
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
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]
Z=1
)
Z,
E
( $
@
H=
!
Φ
$
%'
-
-
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.
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].
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
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].
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
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.
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].
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
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
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.
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.
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.
Electrons
Material a b c
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.
Material a b c a b c
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 .
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 .
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.
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)
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
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.
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].
153
154 Sources of Radiation Chap. 5
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
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].
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.
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
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].
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.
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.
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].
B4
ωK = , (5.4)
1 + B4
where the parameter B is given by
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
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.
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.
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
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.
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
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
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 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
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
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
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.
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.
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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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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Rockville, MD: U.S. Department of Health and Human Services, book, Silver Springs, MD: Scinta Inc., 1992.
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TRUBEY, D.K., M.J. BERGER, AND J.H. HUBBELL, “Photon Cross
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Chapter 6
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.
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
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.
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
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
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
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
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.
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
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
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.
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
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
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
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.
1
N
891
x= xi = = 29.7.
N i=1 30
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 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.
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,
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.
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!
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)
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).
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.
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
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!
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.
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
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.
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
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
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
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
Figure 6.14. The standard normal PDF of Example 6.11, showing the
probability region between 2.5 and ∞.
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
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.
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.
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
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
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
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
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
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
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),
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)
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
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
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
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
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 .
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
N 1/2
x 1
σ(x) = = x̂i . (6.90)
N N i=1
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
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
%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
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.
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
" #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
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
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
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.
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.
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 6.25. 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.
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.
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.
!
!"! !
# $!
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?
54, 89, 64, 102, 90, 78, 56, 74, 88, 42,
70, 94, 50, 82, 100, 64, 72, 78, 58, 76
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?
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:
and the following background measurements were taken over ten-minute periods each:
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
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.
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
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.
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
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
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)
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]).
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.
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
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.
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.
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)].
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 ).
Figure 7.11. Comparison of extendable dead time and approximations from Eq. (7.35) and
Eq. (7.37).
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)
Substitution of this result into Eq. (7.35) gives another approximation for nτ , namely
gτ
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
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
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
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
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
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
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
1
τ= −B − B 2 − 4AC , (7.53)
2A
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:
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 .
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
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
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
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
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 .
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.
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
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.
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
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
8 The common notation refers to the diameter and length of a right straight cylinder.
270 Source and Detector Effects Chap. 7
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
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]
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
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
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
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
(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.
(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
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.
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
q
segment of irregular
surface = DAI
r
q
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.
%
Qi Qtotal
E •n̂ dAS = E •n̂ dS = i
= . (8.5)
AS S o o
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
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.
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
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
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
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.
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.
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.
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].
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
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−
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
In the present analysis, VA = VB = Q3 = 0 and the above general relation reduces to
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
stationary electron-ion
space charge pairs
g-ray
A V+
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + -+ + + + + + + + + +
+ + + + + + + +
++ ++ +- + + + + + + + +
- +
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+++ +++- ++- +
+
+
+
+
+
+
+
+
+
+
+
+
+
+
+
A
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + +
+ + + + + + + + + + + + + + + + + + + B
x
0 x1 x0 x2 d
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
The sum of the charge and its resulting induced charges must equal zero, i.e.,
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.
V+
D = s E, (8.63)
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
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 ,
V2 = (x2 − x1 )E2 = d2 E2 ,
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
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
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−
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.
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
r1 r2 r1 − r2
ΔQ = qNo . (8.85)
r1 r2 r1 − r2
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
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.
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
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.
9.2.1 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].
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
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
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
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
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.
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
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 9.7. 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].
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
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.
transfer to occur between Ar+ and CH4 , but not the reverse exchange. Hence,
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.
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)
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)
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 9.4. 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.
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
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,
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
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
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)
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)
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
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),
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.
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
−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.
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
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
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.
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.
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.
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.
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
center electrode
voltage i
supply current center
_ meter
+ electrode
gas-filled chamber virtual ground
Side View End View
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.
9.5.4
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.
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
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
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 - - - - - - - - -
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.
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
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
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.
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).
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?
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HERZENGBERG, A., “Attachment of Slow Electrons to Oxygen ters, New York: McGraw-Hill, 1949.
Molecules,” J. Chem. Phys., 51, 4942–4950, (1969).
RUTHERFORD, F.R.S. AND H. GEIGER, “An Electrical Method
HUK, M., P. IGO-KEMENES, AND A. WAGNER, “Electron Attach- of Counting the Number of α-Particles from Radio-active Sub-
ment to Oxygen, Water, and Methanol in Various Drift Chamber stances,” Proc. of the Royal Society of London A, 81, 141–161,
Gas Mixtures,” Nucl. Instrum. Meth., A267, 107–119, (1988). (1908).
354 Gas-Filled Detectors: Ion Chambers Chap. 9
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Drift Chambers, CERN 77-09, Geneva, 1977. schen Molekularbewegung und der Suspensionen,” Annalen der
SAULI, F., Gaseous Radiation Detectors, Cambridge: Cambridge Physik, 326, 756-780, (1906).
University Press, 2014. TOWNSEND, J.S., “The Diffusion of Ions in Gases,” Phil. Trans.
SCHULTZ, G. AND J. GRESSER, “A Study of Transport Coeffi- of the Royal Society A, 193, 129–151, (1900).
cients of Electrons in Some Gases Used in Proportional and Drift
WILKINSON, D.H., Ionization Chambers and Counters, Cam-
Chambers,” Nucl. Instrum. Meth., 151, 413–431, (1978).
bridge: University Press, 1950.
SHARPE, J., Nuclear Radiation Detectors, London: Methuen &
Co., 1964. WILSON, C.T.R.,“On an Expansion Apparatus for making Visi-
ble the Tracks of Ionising Particles in Gases and some Results
SHULTIS, J.K. AND R.E. FAW, Radiation Shielding, La Grange
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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)
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.
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.
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
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
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
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
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
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)
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.
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
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.
ln M c
= S d−1 + K (10.45)
aP Sa d−1 a
c K
Gas d
(mPa)d−1 V−d V−1
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.
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.
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)
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%.
Table 10.7. Ionization and excitation data for several gases. Data
from [Christophorou 1971; Rice-Evans 1974].
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
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
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
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
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.
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.
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.
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
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
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
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
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],
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
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
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
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].
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
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).
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
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
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).
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.
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.
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
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].
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
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.
window and
drift cathode
electric
gas field lines (a)
region
substrate
electric
gas field lines (b)
region
substrate
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.
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.
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.
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 → ∞.
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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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].
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
region
LLD ergetic electrons lose energy, through bremsstrahlung,
recombination, or de-excitation, processes that lead to
(log scale)
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
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.
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.
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
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.
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
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.
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
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
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.
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.
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)
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.
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.
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
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].
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
REFERENCES
BARSUTO, E., J. DE URQUIJO, I. ALVAREZ, AND C. CISNEROS, LUDLUM MEASUREMENTS, INC., Ludlum Model 44-38 Beta-
“Mobility of He+ , Ne+ , Ar+ , N+ + +
2 , O2 , and CO2 , in their Par- Gamma Detector, Product Manual, 2013b.
ent Gas,” Phys. Rev. E, 61, 3053–3057, (2000).
LUDLUM MEASUREMENTS, INC., Ludlum Model 44-9 Alpha, Beta,
BRADT, H., P.C. GUGELOT, O. HUBER, H. MEDICUS, P. Gamma Detector, Product Manual, 2014a.
PREISWERK, AND und P. SCHERRER, “Empfindlichkeit von LUDLUM MEASUREMENTS, INC., Ludlum 44-9 Compensation Fil-
Zählrohren mit Blei-, Messing und Aluminiumkathode für γ- ter Design, Internal Report 54992, 2014b.
Strahlung im Energieintervall 0.1 MeV bis 3 MeV,” Helv. Phys.
Acta, 19, 77–90, (1946). MONTGOMERY, C.G. AND D.D. MONTGOMERY, “The Discharge
Mechanism of Geiger-Mueller Counters,” Phys. Rev., 57, 1030–
EMERY, E.W., “Geiger Müller and Proportional Counters,” Radi- 1040, (1940).
ation Dosimetry II, Ch. 10, F.H. ATTIX AND W.C. ROESCH,
Eds., New York: Academic Press, 1966. MUNSON, R.J. AND A.M. TYNDALL, “The Mobility of Positive Ions
in Their Own Gas,” Proc. Royal Soc. London A177, 187–191,
GEIGER, H. AND W. MÜLLER, “Elektronenzhlrohr zur Messung (1941).
Schwchster Aktivitten,” Die Naturwissenschaften, 16, 617–618,
(1928a). PRESENT, R.D., “On Self-Quenching Halogen Counters,” Phys.
Rev., 72, 243–244, (1947).
GEIGER, H. AND W. MÜLLER, “Das Elektronenzhlrohr,” Phys.
Zeitschrift, 29, 839–841, (1928b). PRICE, W.J., Nuclear Radiation Detection, 2nd. Ed., New York:
McGraw-Hill, 1963.
GEIGER, H. AND W. MÜLLER, “Technische Bemerkungen zum
Elektronenzhlrohr,” Phys. Zeitschrift, 30, 489–493, (1929a). RUTHERFORD, E. AND H. GEIGER, “An Electrical Method of
Counting the Number of a Particles from Radioactive Sub-
GEIGER, H. AND W. MÜLLER, “Demonstration des Elektronen- stances,” Proc. Royal Society of London, Series A, 81, 141–161,
zhlrohrs,” Phys. Zeitschrift, 30, 523, (1929b). (1908).
Geiger-Müller Tubes, Croydon, UK: Centronic, LTD., 2014. SHARPE, J., Nuclear Radiation Detectors, London: Methuen &
Co., 1964.
KORFF, S.A., Electron and Nuclear Counters—Theory and Use,
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
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.
423
424 Review of Solid State Physics Chap. 12
+
basis
lattice
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.
Square Rectangular
b
-1
tan (a/b)
Centered Rectangular
Oblique
Hexagonal
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
a a
a
Hexagonal
(P)
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.
Table 12.1. Conditions for the 7 crystal systems and 14 Bravais lattices.
three-dimensional lattice. Lattice planes can be defined by Miller indices1 . To describe a single plane, the
following procedure is used:
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
b
a equivalent directions are designated by triangular brackets, hkl.
{
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.
a∗ •b = a∗ •c = b∗ •a = b∗ •c = c∗ •a = c∗ •b = 0. (12.8)
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
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.
band gap
band gap
band of energy states
band gap
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
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.
A + B = C + D. (12.16)
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
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
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
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
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
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
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
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
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
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
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.
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.
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)
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
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
split-off split-off
band band
(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],
2π
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
ky
kz
3p
a
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
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
split-off band
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
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
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.
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
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
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
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,
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
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.
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.
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.
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
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
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
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
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
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
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.
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
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
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].
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].
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].
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
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
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)
+
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
NA− − ND
+
p=2 NA− NA when NA ND . (12.148)
2
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
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
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
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
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
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.
EC − EDD
NC (NDD − 1) exp −
kT
ngDD . (12.176)
(NA − ND )
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
V(x)
I II III IV
V(x)
V0
I II III
V=0 V0
a
-V0
-a x=0 -a 0 a
3. For a cubic unit cell, find the angles between the normals to the pairs of planes defined by the following
Miller indices
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
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.
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
Table 13.1. Widely used inorganic scintillator materials with some of their properties.
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.
E
excited
ground
D
D’
hwe
excitation emission
E2
B Sehwe
hnin C
E1 hnout
E0
hwg
E lmax1 lmax2
Sghwg
Wavelength
A D Qe0 Q
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,
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
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
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,
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.
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,
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,
1.5 1.05
1.4
1.3 ideal
1.00 performance
1.2
Electron Response
Electron Response
(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
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,
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
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]
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.,
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)
N̄
11 These factors affecting PMT performance are explained in Chapter 14.
498 Scintillation Detectors and Materials Chap. 13
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
+
- - - - - -
+
- - h+ - - - -
e-
+
- h+
+ e- - - - e- e-
+
- + e- - - - - -
+
e-
- - - e- -
+
+
e-
- - - - - - -
+
+
M-center F’-center F-center
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
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.
[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.
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- !
#!
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
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
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-
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
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.
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
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
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
!
Li glasses are shown in Fig. 13.21. The decay times gen- "
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].
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.
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
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.
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
(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.
Plastic
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)
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
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].
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.
Naphthalene C10 H8
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.
Table 13.5. Chemical Formulas and Structures of a Few Organic Liquid Scintillation Fluors (solutes).
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.
CH 3
Pseudocumene C6 H3 (CH3 )3 1.12
H3C CH 3
CH 3
Toluene C7 H 8 CH 3 1.00
CH3
Ethylbenzene C8 H10 0.96
H3C CH3
H3C
CH3
n-Butylbenzene C10 H14 0.88
Benzene C6 H 6 0.85
CH 3
CH 3
CH 3
p-Cymene CH3 C6 H4 CH(CH3 )2 0.80
H3C
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
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
unquenched highly
quenched unquenched
Counts
Counts
quenched (a) (b)
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
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
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
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.
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
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.
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].
large, fast, and proportional detectors needed for the detection and energy spectroscopy of heavy ions, gas
scintillation detectors may be a good choice.
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.
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.
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.
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
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
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?
References 557
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Chapter 14
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.
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
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
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.
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
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.
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),
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]
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
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
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.
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
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
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
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 14.12. 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
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
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.
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
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
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,
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
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
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.
Table 14.7. Properties of some common dynode designs. After Hamamatsu [2007].
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
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
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
dynode 1 50
equipotential
lines
semitransparent 80
photocathode
100
125
dynode 4
dynode 2
0 0
200
400
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
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
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
and the secondary emission factor for the same dynode is defined as
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
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
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.
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
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
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
2 σt2 kV α
σtt = σ12 + , (14.68)
(kV α − 1)2
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.
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
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
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,
where G is the gain and tA is the anode rise time. Conforming to the recommendation that ileak /iA ≥ 100,
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
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
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].
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
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.
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
p+
p p p
n
n+
p+ SiO2 n+
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)
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
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,
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Chapter 15
Basics of Semiconductor
Detector Devices
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.
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 .
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.
βen NT
Ren = βen NT fF D (ET ) = , (15.8)
ET − EF
1 + exp
kT
[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
ET − EC
βen = βcn NC exp . (15.10)
kT
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
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.
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
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
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.
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.
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
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.
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
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
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
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 )
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
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
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
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.
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
E E E
xp 0 xi xn xp xp 0 xn xp 0 xn xn
(a)
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.
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 )
which is wider than the ν region. Hence, in the second case the diode is fully depleted with W = 450
microns.
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
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
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
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
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.
_ EC +
EFsn EFs
EV
Carrier generation-recombination
Figure 15.20. Energy band diagram for an n-type Schottky contact under
reverse bias.
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
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
(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
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
(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
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 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 (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
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)
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.
qcs qcs
qfs qfm EC
qfm qfs
EC EFs
EFm EFm
EFs EV
EV
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
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.
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.
9 μn s θAV 2
i= (15.158)
8 W3
where θ is the fraction of injected charge that is
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 .
A photoconductor consists of a semiconductor material upon which ohmic contacts have been applied.
For pure (intrinsic) semiconductors, the conductivity can be described by
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)
hν
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
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.
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.
15.4.1 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
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
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].
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.
_ _
+ +
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
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)
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
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
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 .
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.
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
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
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)
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
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.
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
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.
dN
dQ
+V +V
1 2
1 2 0 Qo
low mt high mt dN
dQ
3 -V -V 4
4
3
0 Qo
∇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.
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
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.
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?
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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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”,
705
706 Semiconductor Detectors Chap. 16
Table 16.1. Chronological initial exploration dates as radiation detectors for selected semiconductors.
Common
Semiconductor Year Reference
Abbreviation
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.
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 )
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.
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
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.
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.
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 ,
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
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
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
5 Klein [1968] lists Ge, Si, GaAs, InP as the sources of data.
712 Semiconductor Detectors Chap. 16
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
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.
16.2.7 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 .
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
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
largely unsuccessful. Regardless, a section in Chapter 17 is reserved for discussion on these types of neutron
detectors.
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
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
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
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 metallization
bottom surface readout
electrodes
bottom oxide
electrodes s
on
n-type junctions cti
jun
e
p-type Si material typ
p-
metallization
oxide
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 16.17. (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
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
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
The maximum charge that can be stored in a single pixel is described by [Schroder 1984] as
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
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
Qmax = −Co (VG − VT ) = (1.73 × 10−8 F cm−2 )(10 V)(2 × 10−3 cm)2 = 6.9 × 10−13 C.
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+ 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.
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
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
log of concentration
ND
log of concentration
surface
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
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
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
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.
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.
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
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
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
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)
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
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
LN2
molecular
sieve
“superinsulation” in vacuum
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
HPGe
crystal
cold finger
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.
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
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
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
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
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.
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].
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,
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].
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.
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
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
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
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].
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
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
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
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
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.
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
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
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
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
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.
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.
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.
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.
References 799
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Chapter 17
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.
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
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
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].
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,
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
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).
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
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.
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%,
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.
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
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.
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
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
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,
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 ]
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
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
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
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
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].
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
Li foil
either reaction
C product can
enter gas
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
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.
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.
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].
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).
*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
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.
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
[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.
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.
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
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
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].
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,
Consequently, if hkl are all even or are all odd, then Fhkl = 4b. However, if hkl is mixed odd and even, then
Fhkl = 0.
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
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)
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.
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.
reference
detector
(a)
neutron beam
reference
test detector detector
(b)
neutron beam
reference
empty detector shell detector
(c)
neutron beam
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.
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%]
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
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 .
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.
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 .
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
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.
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.
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
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
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.
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.
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,
without significant Doppler broadening, the fast self-shielding factor for a thin foil without appreciable
scattering can be approximated by [Profio 1976]
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)
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.
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.
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.
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
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].
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
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.
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
moderator
collimator collimator
shield detector
d
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 .
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.
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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Chapter 18
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
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,
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,
which indicates that a maximum of 64% of the neutron energy can be transferred to a 4 He nucleus in a
single scatter.
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.
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
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
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
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
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
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].
paraffin paraffin
B2O3
paraffin paraffin
Al sleeve
1” diameter holes
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.
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].
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.
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
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
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].
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 18.17. 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].
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
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
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.
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
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
(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
effect of
statistical
fluctuations
(c) (d)
Channel Number (Energy) E0 Channel Number (Energy) E0
(e) (f)
Channel Number (Energy) E0 Channel Number (Energy) E0
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
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
!"
Figure 18.23. Fast neutron reaction cross sections for 12 C. Data are from
[ENDF VIII 2018].
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
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
neutrons
neutrons
gamma rays
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].
! " !" #
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)
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).
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].
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.
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/
En + 0.764 MeV
full energy
elastic scatter peak
recoil continuum
0.75 En
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
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
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
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.
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.
Here φ(E) is the energy dependent flux at the point of interest and the response function is
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.
Likewise the cover cross section is a constant σ c over each energy interval. Thus for the k iteration
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
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 )
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
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.
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
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
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
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
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
systems, the glow curve is displayed. Because the PMT &'$%() & * # $%
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
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-
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
&'()*+
&,*+-.
region
supralinear
region
linear
region
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)
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.
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
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
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
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
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
!
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
!"
!
!#
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.
!
!
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
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
#
!"
!"
#$%&
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.
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.,
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
∗
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 )
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 .
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
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
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.
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.
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
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.
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
Density
Density
0.1
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
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
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.
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.
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
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
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
# $ %" &
2
)
! "
!
1!
%
0
/
.
-
' ' ( ) % * % + + ,
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
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.
Table 19.3. Relative sensitivity of various track etch materials. From Fleischer et al. [1975].
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
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.
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].
_
+++
+
+++++ +++
+
++++++-+
-++-+--++ +++++
--- ----- --
---------------- ++++ +
-
-++-++ --++ -+
-- ----- -- ++
-
+++
+
+++++ ---------+++-+------ + ++ +
++++++-+ - +++++++++++ +++
-++-+--++
--- ----- -- -+ + +
++
--- ----- -- +
---------------- -++-+--++
-
++-++
-----------------
--++ -+
-
--- ----- -- +
+++
+
+++++ --------+-+------- + +
++++ - ++++++++++ +++
++-+
-++-+--++
--- ----- --
---------------- 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
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
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.
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.
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].
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.
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
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
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].
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
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)
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.
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 .
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.
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.
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.
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.
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-
! "#$%
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).
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.
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?
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
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.
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
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
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
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
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)
C(n i)
integral pulse
height spectrum
Counts
differential pulse
height spectrum
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).
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
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,
- 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.
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.
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.
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.
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.
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
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
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
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
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
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
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
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
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
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.
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
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.
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.
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
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
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
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.
With S = N = 6 and all σi = 1, the set of linear fitting equations Eqs. (20.47) becomes
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 .
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
∂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.
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.
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
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
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
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
∂ 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
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
1
δal = βl or λαll δal = βl (20.85)
λαll
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
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
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
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
(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
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.
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
• 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.
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
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].
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.
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.
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)
Eγ
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
From Eq. (20.105) the continuous channel for the maximum 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
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.
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
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
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
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)
Eγ
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)
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
,-.&'/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].
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).
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
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.
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)
Eγ
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
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.
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
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
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.
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
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
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
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.
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.
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-
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
# $ ! " $ % !"#
$%& ! "# %&' !"#$
$ % ! "# $ % !"#
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
0
0 2 4 6 8 10
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].
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].
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
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.
!
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
!
!
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
0.75NH
DH DL
2
DH DL
2 DH 2
NV 2
0.1NL
DS
HS H L LS
Table 20.3. Summary of SSB detector spectral metrics for Fig. 20.41.
252 Cf 235 U
(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).
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.
7. Show that fitting Eq. (20.104) to NE , NF and NP the parameters in the quadratic fit are
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
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
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
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 21.2. 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
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.
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
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.
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
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.).
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.
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.
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.
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.
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
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
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.
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.
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.
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.
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
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.
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)
2μ
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 .
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.
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.
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).
REFERENCES
BEVELACQUA, J.J., Health Physics in the 21st Century, Wein- MCNP6, MCNP6 User’s Manual, LA-CP-13-00634, Los Alamos
heim: Wiley-VCH, 2008. National Laboratory, 2013.
BRODZINSKI, R.L., D.P. BROWN, J.C. EVANS, W.K. HENSLEY, MORGAN, K.Z., “History of Damage and Protection from Ioniz-
J.H. REEVES, N.A. WOG- MAN, F.T. AVIGNONE III, AND H.S. ing Radiation,” in Principles of Radiation Protection,” K.Z.
MILEY, “An Ultralow Background Germanium Gamma-Ray MORGAN AND J.E. TURNER, Eds., New York: Wiley, 1967.
Spectrometer,” Nucl. Instr. Meth., A239, 207–213, (1985).
NCRP, Natural Background Radiation in the United States, Re-
CAMP, D.C., C. GATROUSIS, AND L.A. MAYNARD, “Low Back- port 45, National Council on Radiation Protection and Measure-
ground Ge(Li) Detector Systems for Radioenvironmental Stud- ments, Washington, DC, 1975.
ies,” Nucl. Intru. Meth., 117, 189-211, (1974).
NCRP, Guidance on Radiation Received in Space Activities, Re-
CASE, K.M., F. DE HOFFMANN, AND G. PLACZEK, Introduction port 98, Washington, DC: National Council on Radiation Pro-
to the Theory of Neutron Diffusion, Vol. I, Los Alamos, NM: tection and Measurements, 1989.
Los Alamos Sci. Lab., 1953.
NUDAT, Nuclear Structures and Decay Data, v. 2.7, National Nu-
DEWARAJA, Y., Z. HE, R.F. FLEMING, D.K. WEHE, S.V. GURU,
clear Data Center, Brookhaven National Laboratory. Available
J.C. FERREIRA, AND R.H. FLEMING, “A Position Sensitive β-γ
at http://www.nndc.bnl.gov/; accessed July 2017.
Coincidence Technique for Multiplexed Gamma Spectrometry of
Many Small Samples,” Nucl. Instrum. Meth., A353, 588–592, RIZZACASSA, P., “Nuclear Instruments and Methods in Physics Re-
(1994). search Section B: Beam Interactions with Materials and Atoms,”
EIESENBUD, M., Environmental Radioactivity, 3rd Ed., Orlando, Nucl. Instru. Meth., B17, 519–523, (1986).
Fl: Academic Press, 1987. SATO T., H. YASUDA, K. NIITA, A. ENDO, AND L. SIHVER, “Devel-
EXPACS ver. 4.0; T. SATO, “Analytical Model for Esti- opment of PARMA: PHITS Based Analytical Radiation Model
mating the Zenith Angle Dependence of Terrestrial Cos- in the Atmosphere,” Radiat. Res., 170, 244-259 (2008).
mic Ray Fluxes,” PLOS ONE, 11(8): e0160390. From SATO T. AND K. NIITA, “Analytical Functions to Predict Cosmic-
https://phits.jaea.go.jp/expacs/, accessed June 2018. Ray Neutron Spectra in the Atmosphere,” Radiat. Res., 166,
FAW, R.E. AND J.K. SHULTIS, Radiological Assesssment: Sources 544-555 (2006).
and Exposures, Am. Nucl. Soc., LaGrange Park, IL, 1999. SHULTIS, J.K. AND R.E. FAW, Radiation Shielding, Lagrange
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-
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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
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EXO-200,” Nucl. Instru. Meth., A591, 490–504, (2008). 2537–2586, (1994).
Chapter 22
Nuclear Electronics
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.
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.
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.
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.
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
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
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.
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.
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
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)
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.
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.
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.
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:
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
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
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.
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
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 .
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
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
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)
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
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.
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.
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
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
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)
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.
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].
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.
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.
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
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
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
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.
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
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).
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
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.
(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
22.3.5 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)
q̄
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)
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)
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
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
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.
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.
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 .
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
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.
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
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].
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.
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],
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
delay
line
timing gate
preamplifier amplifier delay 1
discriminator
detector MCA
coincidence counter/
source
analyzer display
detector
timing
preamplifier amplifier delay 2
discriminator
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.
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
detector
amplifier timing
preamplifier delay
discriminator
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.
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
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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
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G G
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.