In view of the rapid growth in both experimental and theoretical studies of multiphoton processes and multiphoton spectroscopy of atoms, ions and molecules in chemistry, physics, biology, material sciences, etc., it is desirable to publish an Advanced Series that contains review papers readable not only by active researchers in these areas, but also by those who are not experts in the field but who intend to enter the field. The present series attempts to serve this purpose. Each review article is written in a self-contained manner by the experts in the area so that the readers can grasp the knowledge in the area without too much preparation.The topics covered in this volume include “Ultrafast Photochemical Dynamics in Solution Studied by Femtosecond Time-Resolved Fluorescence Spectroscopy: Involvement of Highly Excited States”, “Spectral Selective Studies of Molecular Doped Solids and Applications”, “From Multiphoton to Tunnel Ionization”, “Cluster Dynamics in Intense Laser Fields”, and “Molecular Theory of Sum-Frequency Generation and its Application to Study Molecular Chirality”. It is hoped that the collection of topics in this volume will be useful not only to active researchers but also to other scientists in biology, chemistry, materials science and physics.This book has been selected for coverage in:• CC / Physical, Chemical & Earth Sciences• Index to Scientific Book Contents® (ISBC) Preface CONTENTS 1 Ultrafast Photochemical Dynamics in Solution Studied by Femtosecond Time-Resolved Fluorescence Spectroscopy: Involvement of Highly Excited States 1. Introduction 2. Apparatus and Analysis 3. Tetracence: A Prototype 4. Retinal: Cascaded Electronic Relaxation 5. 7-Azaindole Dimer: Excited-State Double Proton Transfer 6. trans-Azobenzene: Ultrafast Photoisomerization 7. Concluding Remarks Acknowledgment References 2 Spectral Selective Studies of Molecular Doped Solids and Applications 1. Introduction 2. Historical Overview 2.1 Before 1960: the pre-laser age 2.2 1960-1990: entering molecular solid intimacy 2.3 Since 1990: to the ultimate limits 3. Spectrally Selective Molecular Materials for Science and Applications 3.1 Molecular crystals and molecular doped crystals 3.2 Molecular doped polymers 3.3 Molecular doped organic solid solutions 3.4 Molecular doped inorganic solid solutions 3.5 Molecular doped inorganic xerogels 3.6 Molecular doped cryogenic matrices 4. Basic Concepts for Understanding Molecular Doped Solids Spectroscopy 4.1 One molecule interacting with light 4.2 Molecules in a crystal 4.3 Molecules in disordered solid 5. Removing Inhomogeneous Broadening: Inhomogeneous-free Spectroscopies 5.1 Ordered and disordered hosts 5.2 Frequency domain inhomogeneous-free spectroscopies 5.3 Time domain inhomogeneous-free spectroscopies 6. Fundamental: Photodynamics in the (Amorphous) Solid State 6.1 Dephasing 6.2 Spectral diffusion 6.3 Concentration dependence and energy transfer 6.4 Electron-phonon coupling 6.5 External field effects 7. Applications: Taking Advantage of the Inhomogeneous Broadening 7.1 The spectral photographic plate 7.2 Spatio-temporal holography 7.3 Data storage: high-density PSHB optical memories 7.4 Data routing 7.5 Temporal recognition 7.6 Spectral analysis 7.7 Ultrafast pulse shaping 7.8 Prospects: coherent control 8. Conclusion Acknowledgments References Bibliography 3 From Multiphoton to Tunnel Ionization 1. Introduction 2. Laser Induced Breakdown 3. Multiphoton Ionization of Atoms (1964-1978) 4. A Persistent Challenge in the 1960s and 1970s: Tunnel Ionization 5. Some Surprises (1979-1989) 6. Tunnel Ionization using Long and Short Wavelength Lasers 7. Which Tunnel Ionization Formula to Use? Conclusion Acknowledgments References 4 Cluster Dynamics in Intense Laser Fields 1. Introduction 2. Atoms and Molecules in Strong Optical Fields 3. Cluster ionization in Strong Optical Fields 4. Experimental Considerations 5. Ion Dynamics in the Coulomb Explosion Regime 6. Ion Dynamics in the Hydrodynamic Regime 7. Electron Dynamic 8. X-ray Emission 9. Concluding Remarks Acknowledgments References 5 Molecular Theory of Sum-Frequency Generations and its Applications to Study Molecular Chirality Preface 1. Introduction 2. General Consideration 3. Susceptibility Method 4. Molecular Theory of SFG in Dipole Approximation 4.1. Resonance-off-resonance SFG 4.2. Off-resonance-resonance SFG 4.3. Resonance-resonance SFG (double resonance SFG) 4.4. Off-resonance-off-resonance SFG 5. Doubly-Resonant IR-UV SFG 5.1. IR-UV SFG 5.2. UV-IR SFG 5.3. Inhomogeneity effect 5.4. High temperature limit for low frequency modes of IRnon active modes 5.5. Results and discussions 5.6. Numerical simulation and applications 6. Optical Studies on Molecular Chirality Using Linear Circular Dichroism 7. Optical Studies on Molecular Chirality Using SFG 7.1. General cases for SFG 7.2. Electric-dipole contribution 7.3. Electric-dipole and magnetic-dipole contributions 7.4. Applications 7.5. Orientational average 7.6. Applications 8. Investigation of Doubly-Resonant IR-UV-vis SFG of Chiral Molecules in Solutions 8.1. Doubly-resonant SFG 8.2. Doubly-resonant IR-UV-vis SFG 8.3. Non-Condon scheme 8.4. Breakdown of the Born-Oppenheimer approximation 8.5. Band-shape function 9. SFG in Chiral Liquids Near Electronic Resonance 10. Sum-Frequency Vibrational Spectroscopy on Chiral Liquids 11. Discussions 11.1. Near electronic resonant SFG 11.2. Singly-resonant IR-UV SFG 11.3. Doubly-resonant IR-UV SFG 12. Concluding Remarks Appendix References Annotation. In view of the rapid growth in both experimental and theoretical studies of multiphoton processes and multiphoton spectroscopy of atoms, ions and molecules in chemistry, physics, biology, material sciences, etc., it is desirable to publish an Advanced Series that contains review papers readable not only by active researchers in these areas, but also by those who are not experts in the field but who intend to enter the field. The present series attempts to serve this purpose. Each review article is written in a self-contained manner by the experts in the area so that the readers can grasp the knowledge in the area without too much preparation