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剑桥2011年英文原版Theory of Molecular Rydberg States
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Molecular Rydberg states have many unusual properties, lending themselves to a diverse range of experimental applications. This book is designed to unravel the mysteries of molecular Rydberg states that lie beyond the scope of accepted spectroscopic theories. It is the first single-authored text to focus on the application of multi-channel quantum defect theory (MQDT) and ab initio theory to this special class of molecular systems, introducing readers to novel theoretical techniques. The scattering techniques of MQDT are examined, along with a unified description of bound states and fragmentation dynamics. Connections with established spectroscopic theory are also described. The book concludes with an account of the spherical tensor and density matrix theories required for the interpretation of multiphoton experiments. While the main text focuses on physical principles and experimental applications, appendices are used to handle advanced mathematical detail. This is a valuable resource for researchers in chemical, atomic and molecular physics. mark child is a distinguished theoretical chemist and internationally recognised authority on quantum defect theory and its applications to molecular systems. He was Coulson Professor of Theoretical Chemistry at the University of Oxford, a post from which he recently retired. 1 Molecular Rydberg states 1 1.1 The nature of Rydberg states 1 1.2 Organization of the text 7 2 The quantum defect picture 17 2.1 Introduction 17 2.2 Coulomb wavefunctions 18 2.3 Single-channel quantization 25 2.4 Coupled channels 27 3 Ab-initio quantum defects 45 3.1 Traditional quantum chemistry 45 3.2 Constrained ab-initio wavefunctions 52 3.3 The R-matrix matching procedure 54 3.4 The Wigner–Eisbud R-matrix 58 3.5 Variational R-matrix theory 62 3.6 Rydberg–valence interactions 74 3.7 The influence of positive ion dipoles 78 4 Frame transformations and channel interactions 90 4.1 Physical assumptions 91 4.2 Rotational channel interactions 97 4.3 Vibrational channel interactions 105 4.4 Vibronic channel interactions 114 5 Competitive fragmentation 125 5.1 Perturbation model for diatomic species 126 5.2 Diatomic predissociation 129 vii viii Contents 5.3 Dissociative recombination and related phenomena 130 5.4 R-matrix formulation 140 5.5 Vibronically induced dissociative recombination of H+3 148 6 Photo-excitation 157 6.1 Introduction 157 6.2 n-photon discrete absorption 158 6.3 Spherical tensor representation 163 6.4 Spatial selectivity 167 6.5 Resonant two-photon excitation 170 6.6 Multiphoton band structure 171 6.7 Angular momentum decoupling in high Rydberg states 177 6.8 ZEKE intensities 183 7 Photo-ionization 191 7.1 Boundary conditions and cross-sections 192 7.2 The photo-ionization matrix element 195 7.3 Integrated cross-section 199 7.4 Differential cross-section 202 7.5 Fixed molecule angular distribution 215 7.6 Resonant two-photon ionization 219 7.7 Orientation and alignment 226 7.8 Spin polarization 232 8 Manipulating Rydberg states 239 8.1 Rydberg wavepackets 239 8.2 The Stark effect 255 Appendix A MQDT normalization 273 A.1 Open channels 273 A.2 Closed channels 275 Appendix B Alternative MQDT representations 278 B.1 Standard representation 278 B.2 Sine–cos representation 279 B.3 Mixed representation 280 Appendix C Rotational frame transformations 282 C.1 Hund’s cases for diatomic molecules 282 C.2 Parity considerations 284 C.3 Basis functions 285 C.4 Diatomic frame transformations 286 C.5 Asymmetric tops 290 Contents ix Appendix D Optical transition and photo-ionization amplitudes 295 D.1 Discrete absorption amplitudes 295 D.2 Photo-ionization amplitudes 297 D.3 Dipole radial matrix elements and Cooper minima 303 Appendix E Generalized MQDT representation 307 Appendix F Notation 310 F.1 Angular momenta 310 F.2 Reduced matrix elements 310 F.3 Other special brackets 312 Index 314 |
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