i
HANDBOOK OF
RADIOACTIVITY
ANALYSIS
Second Edition
With a foreword by
Dr. Mohamed ElBaradei
Director General
International Atomic Energy Agency
Edited by
Michael F. L’Annunziata
Elsevier Science
TABLE OF CONTENTS
CONTRIBUTORS
ACRONYMS, ABBREVIATIONS, AND SYMBOLS
FOREWORD
PREFACE
1 Introduction: Nuclear Radiation, Its Interaction with Matter and Radioisotope Decay
MICHAEL F. L’ANNUNZIATA
I. Introduction
II. Particulate Radiation
A. Alpha Particles
B. Negatrons
C. Positrons
1. N/Z Ratios and Nuclear Stability
2. Positron Emission versus Electron Capture
D. Beta-particle Absorption and Transmission
E. Internal Conversion Electrons
F. Auger Electrons
G. Neutron Radiation
1. Neutron Classification
2. Sources of Neutrons
a. Alpha Particle-Induced Nuclear Reactions
b. Spontaneous Fission
c. Neutron-Induced Fission
d. Photoneutron (γ,n) Sources
e. Accelerator Sources
f. Nuclear Fusion
3. Interaction of Neutrons with Matter
a. Elastic Scattering
b. Inelastic Scattering
c. Neutron Capture
d. Nonelastic Reactions
e. Nuclear Fission
4. Neutron Attenuation and Cross Sections
5. Neutron Decay
III. Electromagnetic Radiation
A. Dual Nature: Wave and Particle
B. Gamma Radiation
C. Annihilation Radiation
D. Cherenkov Radiation
E. X-Radiation
F. Bremsstrahlung
IV. Interaction of Electromagnetic Radiation with Matter
A. Photoelectric Effect
B. Compton Effect
C. Pair Production
D. Combined Photon Interactions
V. Stopping Power and Linear Energy Transfer
A. Stopping Power
B. Linear Energy Transfer
VI. Radioisotope Decay
A. Half-life
B. General Decay Equations
C. Secular Equilibrium
D. Transient Equilibrium
E. No Equilibrium
F. More Complex Decay Schemes
VII. Radioactivity Units and Radionuclide Mass
A. Units of Radioactivity
B. Correlation of Radioactivity and Radionuclide Mass
C. Carrier-Free Radionuclides
References
2 Gas Ionization Detectors
KARL BUCHTELA
I. Introduction: Principles of Radiation Detection by Gas Ionization
II. Characteristics of gas Ionization Detectors
A. Ion Chambers
B. Proportional Counters
C. Geiger-Mueller Counters
III. Definition of Operating Characteristics of Gas Ionization Detectors
A. Counting Efficiency
B. Energy Resolution
C. Resolving Time
D. Localization
IV. Ion Chambers
A. Operating Mode of Ion Chambers
1. Ion Chambers Operating in the Current Mode
2. Charge Integration Ionization Chambers
3. Pulse Mode Ion Chambers
B. Examples and Applications of Ion Chambers
1. Calibration of Radioactive Sources
2. Measurement of Gases
3. Frisch Grid Ion Chambers
4. Radiation Spectroscopy with Ion Chambers
5. Electret Detectors
6. Fission Chambers
V. Proportional Gas Ionization Detectors
A. Examples and Applications of Proportional Counters
1. Gross Alpha-Beta Counting, Alpha-Beta Discrimination and Radiation Spectroscopy
2. Position-Sensitive Proportional Counters
a. Single-Wire Proportional Counters
b. Multiwire Proportional Counters
c. Microstrip and Micropattern Ionization Counters
d. Low-Level Counting Techniques Using Proportional Gas Ionization Detectors
3. Applications in Environmental Monitoring, and Health Physics
a. Radon in Water
b. Measurement of Plutonium-241
c. Measurement of Iron-55
d. Tritium in Air
e. Radiostrontium
f. Health Physics
VI. Geiger-Mueller Counters
A. Designs and Properties of Geiger-Mueller Counters
1. Fill Gas
2. Quenching
3. Plateau
4. Applications
a. Environmental Radioassay
VII. Special Types of Ionization Detectors
A. Neutron Detectors
1. BF3 Tube Construction
2. Detectors for Fast Neutrons
a. Long Counter
3. Neutron Counting in Nuclear Analysis of Fissile Materials and Radioactive Waste
4. Moisture Measurements
B. Multiple Sample Reading Systems
C. Self-Powered Detectors
D. Self-Quenched Streamer
E. Long-Range Alpha Detectors
F. Liquid Ionization and Proportional Detectors
G. Dynamic Random Access Memory Devices (DRAMs)
References
3 Solid State Nuclear Track Detectors
RADOMIR ILIĆ and SAEED A. DURRANI
I. Introduction
II. Fundamental Principles and Methods of Solid State Nuclear Track Detection
A. Physics and Chemistry of Nuclear Tracks
1. Formation of Latent Tracks
a. Factors Determining the Production of ‘Stable’/Etchable Tracks
2. Visualization of Tracks by Chemical and Electrochemical Etching
a. Chemical Etching (CE)
b. Electrochemical Etching (ECE)
B. Track Detector Types and Properties
1. General Properties
2. Ageing and Environmental Effects
C. Track Evaluation Methods
1. Manual/Ocular Counting
2. Spark Counting
3. Advanced Systems for Automatic Track Evaluation
D. Basics of Measurement Procedures
1. Revelation Efficiency
2. Sensitivity
3. Statistical Errors
4. Background Measurement
5. Calibration and Standardization
III. Measurements and Applications
A. Earth and Planetary Sciences
1. Radon Measurements
a. Response of Detectors to Radon and Radon Daughters
b. Types of Measurement
2. Fission Track Dating
3. Planetary Science
a. Lunar Samples
b. Meteoritic Samples
4. Cosmic Ray Measurements: Particle Identification
B. Physical Sciences
1. Particle Spectrometry
2. Heavy Ion Measurements
3. Neutron Measurements
a. Thermal Neutrons
b. Fast Neutrons
4. Nuclear and Reactor Physics
5. Radiography
6. Elemental Analysis and Mapping
C. Biological and Medical Sciences
1. Radiation Protection Dosimetry/Health Physics
a. Radon Dosimetry
b. Neutron Dosimetry
c. Heavy Ion Dosimetry
2. Environmental Sciences
a. Measurement of Uranium and Radium Concentrations in Water, Milk, Soil, and Plants, etc.
b. Plutonium in the Environment
c. ‘Hot Particle’ Measurements
3. Cancer Diagnostics and Therapy
IV. Conclusion
Acknowledgements
References
4 Semiconductor Detectors
PAUL F. FETTWEIS, JAN VERPLANCKE, RAMKUMAR VENKATARAMAN,
BRIAN YOUNG and HAROLD SCHWENN
I. Introduction
A. The Gas-Filled Ionization Chamber
B. The Semiconductor Detector
C. Fundamental Differences between Ge and Si Detectors
1. The Energy Gap
2. The Atomic Number
3. The Purity or Resistivity of the Semiconductor Material
4. Charge Carrier Lifetime τ
II. Ge Detectors
A. High-Purity Ge Detectors
B. Analysis of Typical γ Spectra
1. Spectrum of a Source Emitting a Single γ Ray with Eγ<1022 keV
2. Spectrum of a Multiple γ-Ray Source Emitting at Least One γ Ray with an Energy ³1022 keV
3. Peak Summation
4. True Coincidence Summing Effects
a. True Coincidence Correction for a Simple Case
b. True Coincidence Correction Using Canberra’s Genie2000 Software
c. True Coincidence Correction Using Ortec’s GammaVision Software
5. Ge-Escape Peaks
C. Standard Characteristics of Ge Detectors
1. Energy Resolution
a. The Electronic Noise Contribution (FWHM)elect and Its Time Behavior
b. Interference with Mechanical Vibrations and with External RF Noise
c. Other Sources of Peak Degradation
d. The Gaussian Peak Shape
2. The Peak-to-Compton Ratio
3. The Detector Efficiency
a. Geometrical Efficiency Factor
b. The Intrinsic Efficiency εi and the Transmission Tγ
c. Relative Efficiency
d. The Experimental Efficiency Curve
e. Mathematical Efficiency Calculations
D. Background and Background Reduction
1. Background in the Presence of a Source
2. Background in the Absence of the Source
a. Man-Made Isotopes
b. Natural Isotopes
3. Background of Cosmic Origin
a. “Prompt” Continuously Distributed Background
b. Neutron-Induced “Prompt” Discrete γ Rays
c. “Delayed” γ Rays
4. Background Reduction
a. Passive Background Reduction
b. Active Background Reduction
E. The Choice of a Detector
1. General Criteria
2. The Germanium Well-Type Detector
3. Limitations to the “Relative Efficiency” Quoted for Coaxial Detectors
4. The Broad Energy Germanium or “BEGe” Detector
III. Si Detectors
A. Si(Li) X-Ray Detectors
B. Si Charged Particle Detectors
1. Alpha Detectors
a. Factors Influencing Resolution and Efficiency
b. Factors Influencing Contamination and Stability
c. Stability of the Detection System
d. The Minimum Detectable Activity (MDA)
2. Electron Spectroscopy and β-Counting
3. Continuous Air Monitoring
a. Light-Tightness and Resistance to Harmful Environments
b. Efficiency
c. Background and MDA Problems in Continuous Air Monitoring
IV. Spectroscopic Analysis With Semiconductor Detectors
A. Sample Preparation
1. Sample Preparation for Alpha Spectrometry
a. Sample Mounting
b. Chemical Separation
c. Preliminary Treatments
2. Sample Preparation for Gamma Spectrometry
B. Analysis—Analytical Considerations
1. Analytical Considerations in Alpha Spectrometry
2. Analytical Considerations in Gamma Spectrometry
a. Peak Location
b. Peak Area Analysis
c. Peak Area Corrections
d. Efficiency Calculation
e. Nuclide Identification and Activity Calculation
References
5 Liquid Scintillation Analysis: Principles and Practice
MICHAEL F. L’ANNUNZIATA and MICHAEL J. KESSLER (deceased)
I. Introduction
II. Basic Theory
A. Scintillation Process
B. Alpha-, Beta- and Gamma-Ray Interactions in the LSC
C. Cherenkov Photon Counting
III. Liquid Scintillation Counter or Analyzer (LSC or LSA)
IV. Quench in Liquid Scintillation Counting
V. Methods of Quench Correction in Liquid Scintillation Counting
A. Internal Standard (IS) Method
B. Sample Spectrum Characterization Methods
1. Sample Channels Ratio (SCR)
2. Combined Internal Standard and Sample Channels Ratio (IS-SCR)
3. Sample Spectrum Quench Indicating Parameters
a. Spectral Index of the Sample (SIS)
b. Spectral Quench Parameter of the Isotope Spectrum or SQP(I)
c. Asymmetric Quench Parameter of the Isotope or AQP(I)
C. External Standard Quench Indicating Parameters
1. External standard Channels Ratio (ESCR)
2. H-number (H#)
3. Relative Pulse Height (RPH) and External Standard Pulse (ESP)
4. Spectral Quench Parameter of the External Standard or SQP(E)
5. Transformed Spectral Index of the External Standard (tSIE)
6. G-Number (G#)
D. Preparation and Use of Quenched Standards and Quench Correction Curves
1. Preparation of Quenched Standards
2. Preparation of a Quench Correction Curve
3. Use of a Quench Correction Curve
E. Combined Chemical and Color Quench Correction
F. Direct DPM Methods
1. Conventional Integral Counting Method (CICM)
2. Modified Integral Counting Method (MICM)
3. Efficiency Tracing with 14C (ET)
4. Multivariate Calibration
5. Other Direct DPM Methods
VI. Analysis of X-Ray, Gamma-Ray, Atomic Electron and Positron Emitters
VII. Common Interferences in Liquid Scintillation Counting
A. Background
B. Quench
C. Radionuclide Mixtures
D. Luminescence
1. Bioluminescence
2. Photoluminescence and Chemiluminescence
3. Luminescence Control, Compensation and Elimination
a. Chemical Methods
b. Temperature Control
c. Counting Region Settings
d. Delayed Coincidence Counting
E. Static
F. Wall Effect
VIII. Multiple Radionuclide Analysis
A. Conventional Dual- and Triple-Radionuclide Analysis
1. Exclusion Method
2. Inclusion Method
B. Digital Overlay Technique (DOT)
C. Full Spectrum DPM (FS-DPM)
D. Recommendations for multiple Radionuclide Analysis
E. Statistical and Interpolation Methods
1. Most-Probable-Value Theory
2. Spectral Deconvolution and Interpolation
a. Spectral Fitting
b. Spectrum Unfolding
c. Spectral Interpolation
3. Multivariate Calibration
IX. Radionuclide Standardization
A. CIEMAT/NIST Efficiency Tracing
1. Theory and Principles (3H as the Tracer)
2. Procedure
3. Cocktail Physical and Chemical Stability
4. Potential Universal Application
5. Ionization Quenching and Efficiency Calculations (3H or 54Mn as the Tracer)
B. 4πβ–γ Coincidence Counting
C. Triple-to-Double Coincidence Ratio (TDCR) Efficiency Calculation Technique
1. Principles
2. Experimental Conditions
X. Neutron/Gamma-Ray Measurement and Discrimination
A. Detector Characteristics and Properties
B. Neutron/Gamma-Ray (n/γ) Discrimination
1. Pulse Shape Discrimination (PSD)
2. Time-of-Flight (TOF) Spectrometry
XI. Microplate Scintillation and Luminescence Counting
A. Detector Design
B. Optical Crosstalk
C. Background Reduction
D. Applications
1. Liquid Scintillation Analysis
2. Solid Scintillator Microplate Counting
3. Scintillation Proximity Assay
4. Luminescence Assays
5. Receptor Binding and Cell Proliferation Assays
E. DPM Methods
F. Advantages and Disadvantages
XII. PERALS Spectrometry
XIII. Simultaneous α/β Analysis
A. Establishing the Optimum PDD Setting
B. α/β Spillover Corrections and Activity Calculations
C. Optimizing α/β Discrimination in PDA
D. Quenching Effects in α/β Discrimination
XIV. Scintillation in Dense (Liquid) Rare Gases
XV. Radionuclide Identification
XVI. Air Luminescence Counting
XVII. Liquid Scintillation Counter Performance
A. Instrument Normalization and Calibration
B. Assessing LSA Performance
C. Optimizing LSC Performance
1. Counting Region Optimization
2. Vial Size and Type
3. Cocktail Choice
4. Counting Time
5. Background Reduction
a. Temperature Control
b. Underground Counting Laboratory
c. Shielding
d. Pulse Discrimination Electronics
6. Conclusions
References
6 Environmental Liquid Scintillation Analysis
GORDON T. COOK, CHARLES J. PASSO, JR., and BRIAN CARTER
I. Introduction
II. Low-Level Liquid Scintillation Counting Theory
A. Sources of Background
B. Background Reduction Methods—Instrument Considerations
1. Enhanced Passive/Graded Shielding
2. Active Guard Detectors
3. Pulse Discrimination Electronics
a. Pulse shape Analysis (PSA)
b. Pulse Amplitude Comparison (PAC)
c. Time-Resolved Liquid Scintillation Counting (TR-LSC)
4. TR-LSC Quasi-active Detector Guards
a. Slow Scintillating Plastic
b. Bismuth Germanate (BGO)
5. Counting Region Optimization
a. Region Optimization Procedures and Requirements Under Constant Quench Conditions
b. Region Optimization Under Variable Quench Conditions
6. Process Optimization
C. Background Reduction Methods — Vial, Vial Holder, and Cocktail Considerations
1. Vials
2. Vial Holders
3. Cocktail Choice and Optimization
D. Background Reduction Methods — Environment
III. Alpha/Beta Discrimination
A. Alpha/Beta Separation Theory
B. Alpha/Beta Instrumentation
1. The PERALS Spectrometer
2. Conventional LS Spectrometers with Pulse-Shape Discrimination
a. Wallac (now PerkinElmer Life and Analytical Sciences)
b. Packard Instrument Co. (now PerkinElmer Life and Analytical Sciences)
c. Beckman Coulter Inc.
C. Cocktail and vial Considerations
1. Cocktail Choice
a. Aqueous-Accepting Cocktails
b. Extractive Scintillators
2. Vial Choice
D. Alpha/Beta Calibration
1. Misclassification Calculations
2. Quenching and Quench Correction of Percentage Misclassification
IV. Analysis of Beta Emitting Radionuclides
A. Tritium (3H)
1. Environmental Occurrence
2. Sample Preparation and Analysis
a. Sample Handling
b. Sample Preparation
c. Sample Purification/Extraction Techniques
d. Reference Background Water
e. Standards
f. Quality Control
g. Quality Assurance
B. Radiocarbon (14C)
1. Environmental Occurrence
2. Sample Preparation and Analysis
a. Sample Preparation
b. Standards (Primarily for 14C Dating)
c. Quality Assurance
d. Calculation of Results and Radiocarbon Conventions
C. Nickel-63 (63Ni)
1. Environmental Occurrence
2. Sample Preparation and Analysis
D. Strontium-89 and Strontium-90/Yttrium-90 (89Sr and 90Sr/90Y)
1. Environmental Occurrence
2. Sample Preparation and Analysis
a. Early LSC Methods
b. Recent LSA Methods
c. Cerenkov Counting Methods
E. Technetium-99 (99Tc)
1. Environmental Occurrence
2. Sample Preparation and Analysis
F. Lead-210 (210Pb) [Bismuth-210 (210Bi) and Polonium-210 (210Po)]
1. Environmental Occurrence
2. Sample Preparation and Analysis
a. Direct Counting by Gamma Spectrometry
b. Indirectly by Measurement of its α-emitting Grand-daughter (210Po)
c. By Indirect Measurement of its β--emitting Daughter (210Bi)
G. Thorium-234 (234Th)
1. Environmental Occurrence
2. Sample Preparation and Analysis
H. Plutonium-241 (241Pu)
1. Environmental Occurrence
2. Sample Preparation and Analysis
V. Analysis of Alpha-Emitting Radionuclides Using Conventional LS Spectrometers
with Pulse Shape Discrimination
A. Gross Alpha Measurements
B. Radium-226 (226Ra)
1. Environmental Occurrence
2. Sample Preparation and Analysis
C. Radon-222 (222Rn)
1. Environmental Occurrence
2. Sample Preparation and Analysis
a. 222Rn Measurements in Air
b. 222Rn Measurements in Water
D. Uranium