Ultrafast Dynamics of Chemical SystemsJ.D. Simon The last decade has witnessed significant advances in the ability to generate short light pulses throughout the optical spectrum. These developments have had a tremendous impact on the field of chemical dynamics. Fundamental questions concerning chemical reactions, once thought to be unaddressable, are now easily studied in real-time experiments. Ultrafast spectroscopies are currently being used to study a variety of fundamental chemical phenomena. This book focuses on some of the experimental and associated theoretical studies of reactions in clusters, liquid and solid media. Many of the advances in our understanding of the fundamental details of chemical reactivity result from the interplay of experiment and theory. This theme is present in many of the chapters, indicating the pervasiveness of a combined approach for eludicating molecular models of chemical reactions. With parallel developments in computer simulation, complex chemical sys tems are being studied at a molecular level. The discussions presented in this book recount many areas at the forefront of "ultrafast chemistry". They serve the purpose of both bringing the expert up to date with the work being done in many laboratories as well as introducing those not directly involved in this field to the diverse set of problems that can be studied. I hope that this book conveys the excitement that both I and the other authors in this volume feel about the field of ultrafast chemistry. John D. Simon 1993 1.D. Simon (ed.), Ultrafast Dynamics of Chemical Systems, vii. |
Contents
1 Introduction to Ultrafast Laser Spectroscopic Techniques Used in the Investigation of Condensed Phase Chemical Reactivity | 1 |
Theory and Experiment | 37 |
3 Ultrafast Electron and Proton Reactivity in Molecular Liquids | 81 |
4 The Dynamics of Anion Solvation in Alcohols | 137 |
Semiconductor Interfaces | 163 |
6 Ultrafast Transient Raman Investigations of Condensed Phase Dynamics | 205 |
Role of Contact Radical Ion Pairs and Solvent Separated Radical Ion Pairs | 223 |
8 The Molecular Basis of Solvent Caging | 235 |
9 Dielectric Continuum Models of SoluteSolvent Interactions | 249 |
10 Analysis of Condensed Phase Photochemical Reaction Mechanisms with Resonance Raman Spectroscopy | 267 |
Solvation at the Single Molecule Level | 289 |
12 Quantum Brownian Oscillator Analysis of PumpProbe Spectroscopy in the Condensed Phase | 327 |
13 Charge Transfer Reactions and Solvation Dynamics | 345 |
383 | |
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absorption spectrum acceptor acetonitrile anion anti-Stokes back transfer band barrier beam benzophenone calculated cation charge distribution charge transfer Chem chemical chemistry cm-¹ continuum CRIP curves decay dependence dielectric dielectric relaxation diffusion dipole dissociation donor electron transfer energy Equation excited experimental experiments femtosecond Figure fluorescence formation frequency friction function geminate recombination H3O+ hydrated electron Hynes infrared initial intensity interaction ion pair ionization kinetics Lett lifetime measured modes molecular motion observed occur optical oxazine PhOH photochemical photodissociation Phys picosecond polarization potential probe pulses proton prototropic species pump-probe radical radical ion Raman Raman spectroscopy rate constant reaction coordinate reactive relative permittivity S₁ sample scale semiconductor signal solid solution solvated electron solvation dynamics solvent cage solvent molecules spectra spectroscopy spectrum SSRIP Stokes studies surface technique theory time-resolved tion transfer parameters transfer reactions transient absorption ultrafast vibrational relaxation water molecules wavelength Zewail