The new nuclear forensics

310 Pages·2015·4.47 MB·English

THE NEW NUCLEAR
FORENSICS
Analysis of Nuclear Materials
for Security Purposes
edited by vitaly fedchenko
The New Nuclear
Forensics
Analysis of Nuclear Materials
for Security Purposes
STOCKHOLM INTERNATIONAL
PEACE RESEARCH INSTITUTE
SIPRI is an independent international institute dedicated to research into
conflict, armaments, arms control and disarmament. Established in 1966,
SIPRI provides data, analysis and recommendations, based on open
sources, to policymakers, researchers, media and the interested public.
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publications of the Institute.
GOVERNING BOARD
Sven-Olof Petersson, Chairman (Sweden)
Dr Dewi Fortuna Anwar (Indonesia)
Dr Vladimir Baranovsky (Russia)
Ambassador Lakhdar Brahimi (Algeria)
Jayantha Dhanapala (Sri Lanka)
Ambassador Wolfgang Ischinger (Germany)
Professor Mary Kaldor (United Kingdom)
The Director
DIRECTOR
Dr Ian Anthony (United Kingdom)

Signalistgatan 9
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Internet: www.sipri.org
The New Nuclear
Forensics
Analysis of Nuclear Materials
for Security Purposes

EDITED BY VITALY FEDCHENKO

OXFORD UNIVERSITY PRESS
2015
1
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United Kingdom
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ISBN 978–0–19–873664–6
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Contents

Preface xiii
Acknowledgements xv
Abbreviations xvi
Glossary xxi
1. Introduction 1
VITALY FEDCHENKO
I. National security policies and the analysis of nuclear 1
materials
II. Nuclear forensic analysis as a collective term 4
III. The applications and purposes of nuclear forensic analysis 7
Box 1.1. Definitions 6
Table 1.1. Applications of nuclear forensic analysis 8
Part I. Nuclear forensic methods
2. The process of nuclear forensic analysis 11
VITALY FEDCHENKO
I. Sample collection and categorization 13
Sample collection 13
Sample categorization 16
II. Sample characterization 19
Material characteristics 19
Measurement techniques and equipment 19
III. Nuclear forensic interpretation 23
Signatures 23
The process of interpretation 25
Libraries, databases and archives 26
Table 2.1. Materials and their forms sampled for nuclear 12
forensic purposes
Table 2.2. Categories of nuclear materials 16
Table 2.3. Categories of radioactive materials other than 17
nuclear materials
Table 2.4. Categories of characteristics of materials or items 18
subject to measurement
Table 2.5. Typical material characteristics categories and 20
measurement technique
Table 2.6. Measurement techniques typical for sample 21
characterization in nuclear forensic analysis
vi THE NEW NUCLEAR FORENSICS
Appendix 2A. Basic facts and definitions related to measurement 34
SOPHIE GRAPE
I. Terms and definitions 34(cid:1)
Accuracy and precision 35(cid:1)
Fundamental aspects of the measurand 36(cid:1)
Statistical distributions 37(cid:1)
Measuring errors 39(cid:1)
II. Assessment of a measurand 40(cid:1)
Currie classification scheme and data interpretation 41(cid:1)
III. Application to counting measurements 45(cid:1)
How good is the fit to data? 46(cid:1)
Figure 2A.1. Graphical representation of the terms accuracy 36
and precision using a dartboard
Figure 2A.2. The normal distribution, the Poisson distribution and 38
Student’s t-distribution with three independent parameters(cid:1)
Figure 2A.3. The standard normal distribution showing the maximum 42
acceptable error of the first kind
3. Inorganic mass spectrometry as a tool of destructive nuclear forensic 47
analysis
KLAUS MAYER, MARIA WALLENIUS, ZSOLT VARGA, MAGNUS HEDBERG AND
NICOLE ERDMANN
I. Thermal ionization mass spectrometry 48(cid:1)
Principle and general description 49(cid:1)
Application of TIMS in nuclear forensics 50(cid:1)
II. Inductively coupled plasma mass spectrometry 52(cid:1)
Principle and general description 52(cid:1)
Determination of elemental composition and impurities 55(cid:1)
Isotope ratio measurements by multi-collector ICP-MS 58(cid:1)
Example of the use of ICP-MS in nuclear forensics 61(cid:1)
III. Secondary ion mass spectrometry 63(cid:1)
Principle and general description 63(cid:1)
Classical safeguards application of uranium particle 63
analysis by SIMS (cid:1)
Examples of forensic application of SIMS analysis 67(cid:1)
IV. Other mass spectrometric techniques 68(cid:1)
Resonance ionization mass spectrometry 69(cid:1)
Accelerator mass spectrometry 73(cid:1)
Figure 3.1. Sample of uranium ore concentrate seized at Rotterdam in 50
2003, after arrival at the nuclear forensics laboratory(cid:1)
Figure 3.2. A typical mass spectrum of the thorium fraction, obtained 56
from confiscated material for age measurement(cid:1)
Figure 3.3. The lead-207 : lead-204 isotope-abundance ratio measured 60
in selected uranium ore concentrate samples
CONTENTS vii
Figure 3.4. The strontium-87 : strontium-86 isotope-abundance ratio 62
of selected uranium ore concentrate samples(cid:1)
Figure 3.5. Scanning electron microscope picture of a conglomerate of 64
uranium particles(cid:1)
Figure 3.6. Vacuum impactor 65(cid:1)
Figure 3.7. A large geometry SIMS instrument 66(cid:1)
Figure 3.8. Plot of individual particle analysis showing uranium-236 67
versus uranium-235 and uranium-234 versus uranium-235 (cid:1)
Figure 3.9. The typical structure of a particle from a nuclear fuel 68(cid:1)
Figure 3.10. Resonance ionization mass spectrometry spectrum of 72
plutonium from a metal plate of natural uranium from the
German nuclear programme of the 1940s (cid:1)
Table 3.1. Nuclear forensic measurement methods 48(cid:1)
Table 3.2. Typical detection limits and precisions of inductively 58
coupled plasma mass spectrometry instruments for fissile
nuclides
4. Gamma spectrometry as a tool of non-destructive nuclear forensic 74
analysis
SOPHIE GRAPE
I. The principle of gamma spectrometry 74(cid:1)
The physics behind gamma spectrometry 74(cid:1)
Electromagnetic interactions with matter 75(cid:1)
Measurement principles 75(cid:1)
II. Gamma spectrometry equipment 77(cid:1)
Detector types 78(cid:1)
III. Ability, demands and limitations of gamma detectors 83(cid:1)
Explanations for the peak width 85(cid:1)
Measurement time 87(cid:1)
Background radiation 89(cid:1)
IV. Special applications of gamma spectrometry 90(cid:1)
Airborne and air-related measurements 90(cid:1)
Underwater measurements 91(cid:1)
Underground experiments 92
Figure 4.1. Example of two Gaussian distributions with the same 84
centroid value but different resolutions (cid:1)
5. Sample characteristics and nuclear forensic signatures 93
KLAUS MAYER, MARIA WALLENIUS AND ZSOLT VARGA
I. Physical characteristics and signatures 93(cid:1)
Metallic uranium and plutonium 94(cid:1)
Fuel pellets 95(cid:1)
Powders and liquids related to the nuclear fuel cycle 99(cid:1)
II. Chemical characteristics and signatures 101(cid:1)
Uranium compounds 102(cid:1)
Plutonium compounds 106(cid:1)
Common non-nuclear chemicals in the fuel cycle 107
viii THE NEW NUCLEAR FORENSICS
III. Elemental characteristics and signatures 109(cid:1)
IV. Isotopic characteristics and signatures 111(cid:1)
Plutonium isotopes 111(cid:1)
Determination of the age of plutonium 113(cid:1)
Uranium isotopes 117(cid:1)
Other important stable isotope ratios 122(cid:1)
Figure 5.1. Uranium and plutonium metal in various shapes 94(cid:1)
Figure 5.2. Metallic cubes made of natural uranium used in the first 95
prototype reactors in Germany and the United States (cid:1)
Figure 5.3. Aircraft counterweight 96(cid:1)
Figure 5.4. Examples of uranium oxide pellets used in nuclear power 96
reactors(cid:1)
Figure 5.5. A uranium fuel pellet, showing dimensions and markings 98(cid:1)
Figure 5.6. Scanning electron microscopy images of the grain 98
morphology of two pellets from different manufacturers (cid:1)
Figure 5.7. Lower magnification scanning electron microscopy images 100
of two samples of uranium ore concentrate (cid:1)
Figure 5.8. Higher magnification scanning electron microscopy images 100
of two samples of uranium ore concentrate(cid:1)
Figure 5.9. Photographs of two samples of uranium ore concentrate 101(cid:1)
Figure 5.10. The Fourier-transform infrared spectroscopy spectra of 102
chemical compounds found in uranium ore concentrate (cid:1)
Figure 5.11. The infrared spectrum recorded for ammonium diuranate 104
from a sample of uranium ore concentrate (cid:1)
Figure 5.12. The measured ion chromatogram for ammonium diuranat 105
from a sample of uranium ore concentrate (cid:1)
Figure 5.13. The rare-earth elemental pattern of various uranium ores 110
and the respective uranium ore concentrates produced(cid:1)
Figure 5.14. The plutonium-240 : plutonium-239 ratio versus the 114
plutonium-242 : plutonium-239 ratio in different reactor
types(cid:1)
Figure 5.15. The variation of main progeny-to-parent nuclide atom 115
ratios for the most important nuclear radionuclides as a
function of time (cid:1)
Figure 5.16. Variation of the thorium-230 : thorium-234 atom ratio in 120
uranium oxide as a function of time (cid:1)
Figure 5.17. Age of uranium samples determined from the uranium- 121
234 : thorium-230 ratio by thermal ionization mass
spectrometry (cid:1)
Figure 5.18. Variation of the thorium-228 : thorium-232 and 122
radium-228 : thorium-232 ratios as a function of time (cid:1)
Figure 5.19. Alpha spectrum of a confiscated nuclear material sample 124
with the presence of trace-level actinides (cid:1)
Figure 5.20. The neodymium-143 : neodymium-144 ratio in uranium ore 125
concentrate samples (cid:1)
Figure 5.21. Observed rainwater delta-oxygen-18 values in Europe 126(cid:1)
CONTENTS ix
Table 5.1. The geometry of pellets used in different types of nuclear 97
reactor
Table 5.2. Examples of non-nuclear components in nuclear material 108(cid:1)
Table 5.3. Plutonium categories and subcategories 112(cid:1)
Table 5.4. Uranium categories 118(cid:1)
Table 5.5. Typical examples of isotopes of impurities investigated in 123
nuclear forensic analysis (cid:1)
6. Radionuclide signatures relevant for post-nuclear explosion 128
environments
LARS-ERIK DE GEER
I. Radiation doses to humans 130(cid:1)
II. Nuclides from an abandoned underground nuclear test site 131(cid:1)
III. Particulate radionuclides relevant for verification of the 133
CTBT (cid:1)
Category 1. Residues of fuel materials 136(cid:1)
Category 2. Non-fission reaction products of fuel materials 139(cid:1)
Category 3. Fission products 141(cid:1)
Category 4. Activation products of non-fuel bomb materials 142(cid:1)
Category 5. Activation products in stemming (filling) 143
materials and rocks surrounding an underground explosion (cid:1)
Category 6. Activation products in the ground below a 144
near-surface atmospheric explosion
Category 7. Activation products in seawater around an 144
underwater or near-sea surface explosion (cid:1)
Category 8. Activation products in air around an 144
atmospheric explosion (cid:1)
Category 9. Activation products deriving from neutron 145
fluence detectors (cid:1)
Category 10. Added tracers 145(cid:1)
Making a final list of CTBT-relevant particulate nuclides 146(cid:1)
IV. Noble gas radionuclides relevant to the IMS of the CTBT 153 (cid:1)
V. Particulate and gaseous nuclides relevant for on-site 154
inspection (cid:1)
Figure 6.1. The CTBTO’s five-level categorization scheme 134(cid:1)
Figure 6.2. A schematic picture of a thermonuclear weapon 136(cid:1)
Table 6.1. Radionuclides relevant for estimating worldwide average 130
effective dose commitments from past nuclear weapon
testing(cid:1)
Table 6.2. The 36 radionuclides relevant for estimating underground 132
inventories at the Mururoa and Fangataufa nuclear test
sites(cid:1)
Table 6.3. The 42 particulate fission products relevant to the 148
International Monitoring System of the CTBT(cid:1)