Nuclear and Radiochemistry

Preface xi Volume 1 1 Fundamental Concepts 1 1.1 The Atom 2 1.2 Atomic Processes 2 1.3 Discovery of the Atomic Nucleus 4 1.4 Nuclear Decay Types 6 1.5 Some Physical Concepts Needed in Nuclear Chemistry 11 1.5.1 Fundamental Forces 11 1.5.2 Elements from Classical Mechanics 12 1.5.3 Relativistic Mechanics 12 1.5.4 The de Broglie Wavelength 14 1.5.5 Heisenberg Uncertainty Principle 15 1.5.6 The Standard Model of Particle Physics 16 1.5.7 Force Carriers 19 Reference 20 Further Reading 20 2 Radioactivity in Nature 23 2.1 Discovery of Radioactivity 23 2.2 Radioactive Substances in Nature 26 References 30 Further Reading 30 3 Radioelements and Radioisotopes and Their Atomic Masses 33 3.1 Periodic Table of the Elements 33 3.2 Isotopes and the Chart of Nuclides 34 3.3 Nuclide Masses and Binding Energies 39 3.4 Evidence for Shell Structure in Nuclei 47 3.5 Precision Mass Spectrometry 49 References 55 Further Reading 55 4 Other Physical Properties of Nuclei 57 4.1 Nuclear Radii 57 4.2 Nuclear Angular Momenta 63 4.3 Magnetic Dipole Moments 65 4.4 Electric Quadrupole Moments 67 4.5 Statistics and Parity 69 4.6 Excited States 70 References 71 Further Reading 71 5 The Nuclear Force and Nuclear Structure 73 5.1 Nuclear Forces 73 5.2 Charge Independence and Isospin 76 5.3 Nuclear Matter 81 5.4 Fermi Gas Model 82 5.5 Shell Model 84 5.6 Collective Motion in Nuclei 94 5.7 Nilsson Model 101 5.8 The Pairing Force and Quasi-Particles 104 5.9 Macroscopic–Microscopic Model 106 5.10 Interacting Boson Approximation 108 5.11 Further Collective Excitations: Coulomb Excitation, High-Spin States, Giant Resonances 110 References 117 Further Reading 117 6 Decay Modes 119 6.1 Nuclear Instability and Nuclear Spectroscopy 119 6.2 Alpha Decay 119 6.2.1 Hindrance Factors 125 6.2.2 Alpha-Decay Energies 126 6.3 Cluster Radioactivity 126 6.4 Proton Radioactivity 129 6.5 Spontaneous Fission 132 6.6 Beta Decay 148 6.6.1 Fundamental Processes 148 6.6.2 Electron Capture-to-Positron Ratios 158 6.6.3 Nuclear Matrix Elements 160 6.6.4 Parity Non-conservation 162 6.6.5 Massive Vector Bosons 164 6.6.6 Cabibbo–Kobayashi–Maskawa Matrix 165 6.7 Electromagnetic Transitions 170 6.7.1 Multipole Order and Selection Rules 172 6.7.2 Transition Probabilities 174 6.7.3 Internal Conversion Coefficients 179 6.7.4 Angular Correlations 183 References 186 Further Reading 187 7 Radioactive Decay Kinetics 189 7.1 Law and Energy of Radioactive Decay 189 7.2 Radioactive Equilibria 191 7.3 Secular Radioactive Equilibrium 193 7.4 Transient Radioactive Equilibrium 196 7.5 Half-life of Mother Nuclide Shorter than Half-life of Daughter Nuclide 197 7.6 Similar Half-lives 198 7.7 Branching Decay 199 7.8 Successive Transformations 200 Reference 202 Further Reading 203 8 Nuclear Radiation 205 8.1 General Properties 205 8.2 Heavy Charged Particles (A ≥ 1) 207 8.3 Beta Radiation 214 8.4 Gamma Radiation 220 8.5 Neutrons 227 8.6 Short-lived Elementary Particles in Atoms and Molecules 232 References 233 Further Reading 234 9 Measurement of Nuclear Radiation 235 9.1 Activity and Counting Rate 235 9.2 Gas-Filled Detectors 239 9.2.1 Ionization Chambers 243 9.2.2 Proportional Counters 244 9.2.3 Geiger–Müller Counters 246 9.3 Scintillation Detectors 248 9.4 Semiconductor Detectors 250 9.5 Choice of Detectors 256 9.6 Spectrometry 259 9.7 Determination of Absolute Disintegration Rates 262 9.8 Use of Coincidence and Anticoincidence Circuits 263 9.9 Low-Level Counting 263 9.10 Neutron Detection and Measurement 264 9.11 Track Detectors 266 9.11.1 Photographic Emulsions and Autoradiography 266 9.11.2 Dielectric Track Detectors 267 9.11.3 Cloud Chambers 268 9.11.4 Bubble Chambers 268 9.11.5 Spark Chambers 269 9.12 Detectors Used in Health Physics 269 9.12.1 Portable Counters and Survey Meters 269 9.12.2 Film Badges 270 9.12.3 Pocket Ion Chambers 270 9.12.4 Thermoluminescence Dosimeters 270 9.12.5 Contamination Monitors 270 9.12.6 Whole-Body Counters 271 Reference 271 Further Reading 271 10 Statistical Considerations in Radioactivity Measurements 273 10.1 Distribution of Random Variables 273 10.2 Probability and Probability Distributions 275 10.3 Maximum Likelihood 282 10.4 Experimental Applications 283 10.5 Statistics of Pulse-Height Distributions 285 10.6 Setting Upper Limits When No Counts are Observed 287 Further Reading 288 11 Techniques in Nuclear Chemistry 289 11.1 Special Aspects of the Chemistry of Radionuclides 289 11.1.1 Short-Lived Radionuclides and the Role of Carriers 289 11.1.2 Radionuclides of High Specific Activity 291 11.1.3 Microamounts of Radioactive Substances 292 11.1.4 Radiocolloids 297 11.1.5 Tracer Techniques 299 11.2 Target Preparation 300 11.3 Measuring Beam Intensity and Fluxes 306 11.4 Neutron Spectrum in Nuclear Reactors 308 11.4.1 Thermal Neutrons 308 11.4.2 Epithermal Neutrons and Resonances 310 11.4.3 Reaction Rates in Thermal Reactors 311 11.5 Production of Radionuclides 311 11.5.1 Production in Nuclear Reactors 311 11.5.2 Production by Accelerators 318 11.5.3 Separation Techniques 324 11.5.4 Radionuclide Generators 329 11.6 Use of Recoil Momenta 331 11.7 Preparation of Samples for Activity Measurements 336 11.8 Determination of Half-Lives 337 11.9 Decay-Scheme Studies 339 11.10 In-Beam Nuclear Reaction Studies 342 References 355 Further Reading 357 Volume 2 12 Nuclear Reactions 361 12.1 Collision Kinematics 362 12.2 Coulomb Trajectories 364 12.3 Cross-sections 368 12.4 Elastic Scattering 372 12.5 Elastic Scattering and Reaction Cross-section 379 12.6 Optical Model 383 12.7 Nuclear Reactions and Models 385 12.7.1 Investigation of Nuclear Reactions 386 12.7.2 Compound-Nucleus Model 386 12.7.3 Precompound Decay 403 12.7.4 Direct Reactions 404 12.7.5 Photonuclear Reactions 407 12.7.6 Fission 407 12.7.7 High-Energy Reactions 418 12.8 Nuclear Reactions Revisited with Heavy Ions 422 12.8.1 Heavy-Ion Fusion Reactions 424 12.8.2 Quasi-fission 434 12.8.3 Deep Inelastic Collisions 440 12.8.4 Relativistic Heavy-Ion Collisions, the Phases of Nuclear Matter 457 References 460 Further Reading 462 13 Chemical Effects of Nuclear Transmutations 465 13.1 General Aspects 465 13.2 Recoil Effects 466 13.3 Excitation Effects 471 13.4 Gases and Liquids 476 13.5 Solids 479 13.6 Szilard–Chalmers Reactions 482 13.7 Recoil Labeling and Self-labeling 484 References 485 Further Reading 485 14 Influence of Chemical Bonding on Nuclear Properties 487 14.1 Survey 487 14.2 Dependence of Half-Lives on Chemical Bonding 488 14.3 Dependence of Radiation Emission on the Chemical Environment 490 14.4 Mössbauer Spectrometry 499 References 504 Further Reading 505 15 Nuclear Energy, Nuclear Reactors, Nuclear Fuel, and Fuel Cycles 507 15.1 Energy Production by Nuclear Fission 507 15.2 Nuclear Fuel and Fuel Cycles 512 15.3 Production of Uranium and Uranium Compounds 517 15.4 Fuel Elements 520 15.5 Nuclear Reactors, Moderators, and Coolants 524 15.6 The Chernobyl Accident 532 15.7 Reprocessing 537 15.8 Radioactive Waste 544 15.9 The Natural Reactors at Oklo 551 15.10 Controlled Thermonuclear Reactors 552 15.11 Nuclear Explosives 554 References 555 Further Reading 555 16 Sources of Nuclear Bombarding Particles 559 16.1 Neutron Sources 559 16.2 Neutron Generators 560 16.3 Research Reactors 561 16.4 Charged-Particle Accelerators 565 16.4.1 Direct Voltage Accelerators 565 16.4.2 Linear Accelerators 568 16.4.3 Cyclotrons 570 16.4.4 Synchrocyclotrons, Synchrotrons 574 16.4.5 Radioactive Ion Beams 576 16.4.6 Photon Sources 577 References 578 Further Reading 579 17 Radioelements 581 17.1 Natural and Artificial Radioelements 581 17.2 Technetium and Promethium 585 17.3 Production of Transuranic Elements 588 17.3.1 Hot-Fusion Reactions 594 17.3.2 Cold-Fusion Reactions 598 17.3.3 48Ca-Induced Fusion Reactions 604 17.4 Cross-sections 606 17.5 Nuclear Structure of Superheavy Elements 610 17.6 Spectroscopy of Actinides and Transactinides 615 17.7 Properties of the Actinides 618 17.8 Chemical Properties of the Transactinides 629 17.8.1 Prediction of Electron Configurations and the Architecture of the Periodic Table of the Elements 630 17.8.2 Methods to Investigate the Chemistry of the Transactinides 632 17.8.3 Selected Experimental Results 653 References 668 Further Reading 671 18 Radionuclides in Geo- and Cosmochemistry 677 18.1 Natural Abundances of the Elements and Isotope Variations 677 18.2 General Aspects of Cosmochemistry 680 18.3 Early Stages of the Universe 681 18.4 Synthesis of the Elements in the Stars 683 18.4.1 Evolution of Stars 684 18.4.2 Evolution of the Earth 686 18.4.3 Thermonuclear Reaction Rates 687 18.4.4 Hydrogen Burning 688 18.4.5 Helium Burning 690 18.4.6 Synthesis of Nuclei with A < 60 690 18.4.7 Synthesis of Nuclei with A > 60 691 18.5 The Solar Neutrino Problem 696 18.6 Interstellar Matter and Cosmic Radiation 704 18.6.1 Interstellar Matter 704 18.6.2 Cosmic Radiation 705 18.6.3 Radionuclides from Cosmic Rays 706 18.6.4 Cosmic-Ray Effects in Meteorites 706 18.6.5 Abundance of Li, Be, and B 707 References 708 Further Reading 708 19 Dating by Nuclear Methods 711 19.1 General Aspect 711 19.2 Cosmogenic Radionuclides 712 19.3 Terrestrial Mother/Daughter Nuclide Pairs 717 19.4 Natural Decay Series 720 19.5 Ratios of Stable Isotopes 723 19.6 Radioactive Disequilibria 724 19.7 Fission Tracks 725 References 726 Further Reading 727 20 Radioanalysis 729 20.1 General Aspects 729 20.2 Analysis on the Basis of Inherent Radioactivity 730 20.3 Neutron Activation Analysis (NAA) 732 20.4 Activation by Charged Particles 736 20.5 Activation by Photons 738 20.6 Special Features of Activation Analysis 739 20.7 Isotope Dilution Analysis 741 20.8 Radiometric Methods 743 20.9 Other Analytical Applications of Radiotracers 745 20.10 Absorption and Scattering of Radiation 745 20.11 Radionuclides as Radiation Sources in X-ray Fluorescence Analysis (XFA) 746 20.12 Analysis with Ion Beams 748 20.13 Radioisotope Mass Spectrometry 752 20.13.1 Resonance Ionization Mass Spectrometry (RIMS) 752 20.13.2 Accelerator Mass Spectrometry (AMS) 757 References 761 Further Reading 763 21 Radiotracers in Chemistry 765 21.1 General Aspects 765 21.2 Chemical Equilibria and Chemical Bonding 765 21.3 Reaction Mechanisms in Homogeneous Systems 767 21.4 Reaction Mechanisms in Heterogeneous Systems 772 21.5 Diffusion and Transport Processes 776 21.6 Emanation Techniques 778 References 781 Further Reading 781 22 Radionuclides in the Life Sciences 783 22.1 Survey 783 22.2 Application in Ecological Studies 784 22.3 Radioanalysis in the Life Sciences 784 22.4 Application in Physiological and Metabolic Studies 786 22.5 Radionuclides Used in Nuclear Medicine 787 22.6 Single-Photon Emission Computed Tomography (SPECT) 789 22.7 Positron Emission Tomography (PET) 790 22.8 Labeled Compounds 790 References 797 Further Reading 797 23 Technical and Industrial Applications of Radionuclides and Nuclear Radiation 801 23.1 Radiotracer Techniques 801 23.2 Absorption and Scattering of Radiation 803 23.3 Radiation-induced Reactions 805 23.4 Energy Production by Nuclear Radiation 807 Further Reading 810 24 Radionuclides in the Geosphere and the Biosphere 813 24.1 Sources of Radioactivity 813 24.2 Mobility of Radionuclides in the Geosphere 816 24.3 Reactions of Radionuclides with the Components of Natural Waters 818 24.4 Interactions of Radionuclides with Solid Components of the Geosphere 823 24.5 Radionuclides in the Biosphere 826 24.6 Speciation Techniques with Relevance for Nuclear Safeguards, Verification, and Applications 832 24.6.1 Redox Reactions, Hydrolysis, and Colloid Formation of Pu(IV) 837 24.6.2 Investigation of the Homologs Th(IV) and Zr(IV) 842 24.6.3 Time-resolved Laser-induced Fluorescence 850 24.6.4 Conclusions 854 References 854 Further Reading 855 25 Dosimetry and Radiation Protection 861 25.1 Dosimetry 861 25.2 External Radiation Sources 864 25.3 Internal Radiation Sources 865 25.4 Radiation Effects in Cell 867 25.5 Radiation Effects in Humans, Animals, and Plants 868 25.6 Non-occupational Radiation Exposure 872 25.7 Safety Recommendations 872 25.8 Safety Regulations 875 25.9 Monitoring of the Environment 879 References 880 Further Reading 880 Appendix 883 Glossary 883 Physical Constants 887 Conversion Factors 889 Relevant Journals 889 Web References 890 Index 891