MODERN NUCLEAR

CHEMISTRY

WALTER D. LOVELAND
Oregon State University

DAVID J. MORRISSEY
Michigan State University

GLENN T. SEABORG
University of California, Berkeley

O WILEY-
INTERSCIENCE
A JOHN WILEY & SONS, INC., PUBLICATION
CONTENTS

PREFACE xv

CHAPTER 1 INTRODUCTORY CONCEPTS 1

1.1 Introduction / 1
1.2 The Atom / 2
1.3 Atomic Processes / 3
1.3.1 Ionization / 3
1.3.2 X-ray Emission / 4
1.4 The Nucleus Nomenclature / 6
1.5 Survey of Nuclear Decay Types / 8
1.6 Modern Physical Concepts Needed in Nuclear Chemistry / 11
1.6.1 Types of Forces in Nature / 11
1.6.2 Elementary Mechanics / 12
1.6.3 Relativistic Mechanics / 13
1.6.4 De Broglie Wavelength, Wave–Particle Duality / 17
1.6.5 Heisenberg Uncertainty Principle / 19
1.6.6 Units and Conversion Factors / 19
1.7 Particle Physics / 20
1.8 Exchange Particles and Force Carriers / 24
Problems / 24
Bibliography / 26

v
Vi CONTENTS

CHAPTER 2 NUCLEAR PROPERTIES 29

2.1 Introduction / 30
2.2 Nuclear Masses / 30
2.3 Terminology / 32
2.4 Binding Energy Per Nucleon / 33
2.5 Separation Energy Systematics / 35
2.6 Abundance Systematics / 36
2.7 Semiempirical Mass Equation / 36
2.8 Nuclear Sizes and Shapes / 42
2.9 Quantum Mechanical Properties / 44
2.9.1 Nuclear Angular Momenta / 44
2.10 Electric and Magnetic Moments / 47
2.10.1 Magnetic Dipole Moment / 47
2.10.2 Electric Quadrupole Moment / 50
Problems / 53
References / 56
Bibliography / 56

CHAPTER 3 RADIOACTIVE DECAY KINETICS 57

3.1 Basic Decay Equations / 58

3.2 Mixture of Two Independently Decaying Radionuclides / 65
3.3 Radioactive Decay Equilibrium / 67
3.4 Branching Decay / 75
3.5 Natural Radioactivity / 77
3.6 Radionuclide Dating / 81
Problems / 87
References / 89
Bibliography / 89

CHAPTER 4 RADIOTRACERS 91
4.1 Introduction / 91
4.2 Design of a Radiotracer Experiment / 92
4.2.1 Basic Design Criteria / 92
4.2.2 Practical Considerations / 95
4.3 Preparation of Radiotracers and Their Compounds / 97
4.3.1 Chemical Synthesis / 99
4.3.2 Biosynthesis / 100
4.3.3 Tritium Labeling / 100
4.3.4 Radiolysis of Labeled Compounds / 101
 CONTENTS Vi I

4.4 Tracing of Physical Process / 101

4.5 Chemical Applications of Tracers / 102
4.6 Isotope Effects / 104
4.7 Biological Applications / 107
4.8 Environmental Applications / 109
4.9 Industrial Use of Radiotracers / 113
4.10 Nuclear Medicine / 113
4.11 Isotope Dilution Analysis / 122
4.11.1 Direct IDA / 122
4.11.2 Inverse IDA / 123
4.11.3 General Comments / 124
4.11.4 Special IDA Techniques / 124
4.12 Radiometric Techniques / 125
Problems / 127
References / 128
Bibliography / 128

CHAPTER 5 NUCLEAR FORCES 129

5.1 Introduction / 129
5.2 Characteristics of the Strong Force / 130
5.3 Charge Independence of Nuclear Forces / 132
Problems / 134
Reference / 135

CHAPTER 6 NUCLEAR STRUCTURE 137

6.1 Nuclear Potentials / 139
6.2 Schematic Shell Model / 140
6.3 Independent Particle Model / 152
6.4 Collective Model / 154
6.5 Nilsson Model / 160
6.6 Nucleus as a Fermi Gas / 163
Problems / 171
References / 174
Bibliography / 174

CHAPTER 7 a DECAY 177
7.1 Energetics of a Decay / 179
7.2 Theory of a Decay / 183
7.3 Hindrance Factors / 192
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7.4 Heavy Particle Radioactivity / 193

7.5 Proton Radioactivity / 195
Problems / 197
References / 198
Bibliography / 198

CHAPTER 8 ß DECAY 199
8.1 Introduction / 199
8.2 Neutrino Hypothesis / 200
8.3 Derivation of Spectral Shape / 203
8.4 Kurie Plots / 207
8.5 ß-Decay Rate Constant / 208
8.6 Electron Capture Decay / 213
8.7 Parity Nonconservation / 214
8.8 Neutrinos / 215
8.9 ß-Delayed Radioactivities / 216
8.10 Double-ß Decay / 217
Problems / 219
References / 220
Bibliography / 220

CHAPTER 9 y-RAY DECAY 221

9.1 Introduction / 221
9.2 Energetics of y Decay / 222
9.3 Classification of Decay Types / 223
9.4 Electromagnetic Transition Rates / 226
9.5 Internal Conversion / 232
9.6 Angular Correlations / 235
9.7 Mössbauer Effect / 241
Problems / 247
References / 248
Bibliography / 248

CHAPTER 10 NUCLEAR REACTIONS 249

10.1 Introduction / 249
10.2 Energetics of Nuclear Reactions / 250
10.3 Reaction Types and Mechanisms / 254
10.4 Nuclear Reaction Cross Sections / 255
 CONTENTS ix

10.5 Reaction Observables / 264

10.6 Rutherford Scattering / 265
10.7 Elastic (Diffractive) Scattering / 268
10.8 Direct Reactions / 270
10.9 Compound Nucleus Reactions / 272
10.10 Photonuclear Reactions / 278
10.11 Heavy Ion Reactions / 279
10.11.1 Coulomb Excitation / 280
10.11.2 Elastic Scattering / 281
10.11.3 Fusion Reactions / 282
10.11.4 Deep Inelastic Scattering / 286
10.11.5 Incomplete Fusion / 286
10.11.6 Reactions Induced by Radioactive Projectiles / 287
10.12 High-Energy Nuclear Reactions / 288
10.12.1 Spallation/Fragmentation / 288
10.12.2 Multifragmentation / 291
10.12.3 Quark–Gluon Plasma / 292
Problems / 293
References / 296
Bibliography / 297

CHAPTER 11 FISSION 299

11.1 Introduction / 299
11.2 Probability of Fission / 302
11.2.1 Liquid Drop Model / 302
11.2.2 Shell Corrections / 304
11.2.3 Spontaneous Fission / 306
11.2.4 Spontaneously Fissioning Isomers / 308
11.2.5 Transition Nucleus / 310
11.3 Fission Product Distributions / 316
11.3.1 Total Kinetic Energy (TKE) Release in Fission / 316
11.3.2 Fission Product Mass Distributions / 316
11.3.3 Fission Product Charge Distributions / 318
11.4 Excitation Energy of the Fission Fragments / 322
11.5 Dynamical Properties of the Fission Fragments / 325
Problems / 329
References / 329
X CONTENTS

CHAPTER 12 NUCLEAR REACTIONS IN NATURE:

NUCLEAR ASTROPHYSICS 331
12.1 Introduction / 331
12.2 Elemental and Isotopic Abundances / 332
12.3 Primordial Nucleosynthesis / 336
12.4 Stellar Evolution / 338
12.5 Thermonuclear Reaction Rates / 342
12.6 Stellar Nucleosynthesis / 344
12.6.1 Introduction / 344
12.6.2 Hydrogen Burning / 345
12.6.3 Helium Burning / 348
12.6.4 Synthesis of Nuclei with A < 60 / 349
12.6.5 Synthesis of Nuclei with A > 60 / 351
12.7 Solar Neutrino Problem / 354
12.7.1 Introduction / 354
12.7.2 Expected Solar Neutrino Sources, Energies,
and Fluxes / 355
12.7.3 Detection of Neutrinos / 357
12.7.4 Solar Neutrino Problem / 359
12.7.5 Solution of the Problem—Neutrino Oscillations / 359
12.8 Synthesis of Li, Be, and B / 361
Problems / 362
References / 363
Bibliography / 363

CHAPTER 13 ANALYTICAL APPLICATIONS OF

NUCLEAR REACTIONS 365
13.1 Activation Analysis / 366
13.1.1 Basic Description of Method / 366
13.1.2 Advantages and Disadvantages of Activation
Analysis / 367
13.1.3 Practical Considerations in Activation Analysis / 368
13.1.4 Applications of Activation Analysis / 372
13.2 Particle-Induced X-ray Emission / 373
13.3 Rutherford Backscattering (RBS) / 376
Problems / 379
References / 380
Bibliography / 380
 CONTENTS Xi

CHAPTER 14 REACTORS AND ACCELERATORS 383

14.1 Nuclear Reactors / 384
14.1.1 Neutron-Induced Reactions / 384
14.1.2 Neutron-Induced Fission / 387
14.1.3 Neutron Inventory / 388
14.1.4 Light Water Reactors / 390
14.1.5 The Oklo Phenomenon / 395
14.2 Neutron Sources / 395
14.3 Neutron Generators / 396
14.4 Accelerators / 397
14.4.1 Ion Sources / 397
14.4.2 Electrostatic Machines / 399
14.4.3 Linear Accelerators / 403
14.4.4 Cyclotrons, Synchrotrons, and Rings / 406
14.5 Charged Particle Beam Transport and Analysis / 412
14.6 Radioactive Ion Beams / 417
14.7 Nuclear Weapons / 421
Problems / 426
References / 427
Bibliography / 427

CHAPTER 15 THE TRANSURANIUM ELEMENTS 429

15.1 Introduction / 429
15.2 Limits of Stability / 429
15.3 Element Synthesis / 431
15.4 History of Transuranium Element Discovery / 438
15.5 Superheavy Elements / 447
15.6 Chemistry of the Transuranium Elements / 449
15.7 Environmental Chemistry of the Transuranium Elements / 457
Problems / 462
References / 463
Bibliography / 464

CHAPTER 16 NUCLEAR REACTOR CHEMISTRY 465

16.1 Introduction / 465
16.2 Fission Product Chemistry / 466
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16.3 Radiochemistry of Uranium / 470

16.3.1 Uranium Isotopes / 470
16.3.2 Metallic Uranium / 470
16.3.3 Uranium Compounds / 470
16.3.4 Uranium Solution Chemistry / 471
16.4 Nuclear Fuel Cycle—The Front End / 472
16.4.1 Mining and Milling / 472
16.4.2 Refining and Chemical Conversion / 475
16.4.3 Enrichment / 475
16.4.4 Fuel Fabrication / 478
16.5 Nuclear Fuel Cycle—The Back End / 479
16.5.1 Properties of Spent Fuel / 479
16.5.2 Fuel Reprocessing / 481
16.6 Radioactive Waste Disposal / 483
16.6.1 Classification of Radioactive Waste / 483
16.6.2 Amounts and Associated Hazards / 484
16.6.3 Storage and Disposal of Nuclear Waste / 485
16.7 Chemistry of Operating Reactors / 492
16.7.1 Radiation Chemistry of Coolants / 493
16.7.2 Corrosion / 493
16.7.3 Coolant Activities / 494
Problems / 494
References / 495
Bibliography / 496

CHAPTER 17 INTERACTION OF RADIATION

WITH MATTER 497
17.1 Introduction / 497
17.2 Heavy Charged Particles (A > 1) / 499
17.3 Electrons / 514
17.4 Electromagnetic Radiation / 518
17.4.1 Photoelectric Effect / 520
17.4.2 Compton Scattering / 522
17.4.3 Pair Production / 524
17.5 Neutrons / 526
17.6 Radiation Exposure and Dosimetry / 530
Problems / 533
References / 535
Bibliography / 535
 CONTENTS Xi i i

CHAPTER 18 RADIATION DETECTORS 537

18.1 Detectors Based an Ionization / 540
18.1.1 Gas Ionization Detectors / 540
18.1.2 Semiconductor Detectors (Solid-State
Ionization Chambers) / 548
18.2 Scintillation Detectors / 558
18.3 Nuclear Track Detectors / 564
18.4 Nuclear Electronics and Data Collection / 565
18.5 Nuclear Statistics / 567
18.5.1 Rejection of Abnormal Data / 574
18.5.2 Setting Upper Limits When No
Counts are Observed / 576
Problems / 576
References / 577
Bibliography / 577

CHAPTER 19 RADIOCHEMICAL TECHNIQUES 579
19.1 Unique Aspects of Radiochemistry / 580
19.2 Availability of Radioactive Material / 584
19.3 Targetry / 584
19.4 Measuring Beam Intensity and Fluxes / 589
19.5 Recoils, Evaporation Residues (EVRs),
and Heavy Residues / 591
19.6 Radiochemical Separation Techniques / 595
19.6.1 Precipitation / 595
19.6.2 Solvent Extraction / 596
19.6.3 Ion Exchange / 599
19.6.4 Extraction Chromatography / 602
19.6.5 Rapid Radiochemical Separations / 602
19.7 Low-Level Measurement Techniques / 603
19.7.1 Introduction / 603
19.7.2 Blanks / 604
19.7.3 Low-Level Counting—General Principles / 605
19.7.4 Low-Level Counting—Details / 605
19.7.5 Limits of Detection / 608
Problems / 609
References / 610
Bibliography / 611
XIV CONTENTS

APPENDIX A FUNDAMENTAL CONSTANTS AND

CONVERSION FACTORS 613

APPENDIX B NUCLEAR WALLET CARDS 617

APPENDIX C PERIODIC TABLE OF ELEMENTS 639
APPENDIX D LIST OF ELEMENTS 641
APPENDIX E ELEMENTS OF QUANTUM MECHANICS 643
INDEX 665