Synopses & Reviews
This textbook presents a systematic and unifying viewpoint for a wide class of nonlinear spectroscopic techniques in time domain and frequency domain. It is directed towards active researchers in physics, optics, chemistry, and materials science, as well as graduate students who enter this complex and rapidly developing field.
Nonlinear optical interactions of laser fields with matter provide powerful spectroscopic tools for the understanding of microscopic interactions and dynamic processes. One of the major obstacles facing researchers in this field, however, is the flood of experimental techniques and terminologies, which create a serious language barrier. The general microscopic correlation function approach to the nonlinear optical response developed in this book is essential for understanding the relationships among different techniques and a comparison of their information content, the design of new measurements, and for a systematic comparison of the optical response of different systems such as dyes in solutions, atoms and molecules in the gas phase, liquids, molecular aggregates and superlatives, and semiconductor nanostructures. The approach is based on formulating the nonlinear response by representing the state of matter by the density matrix and following its evolution on Liouville space. Current active research areas such as femtosecond time-domain techniques, semi-classical and wave-packet dynamics, pulse shaping, pulse locking, exciton confinement, and the interplay of electronic, nuclear and field coherence are emphasized.
The material has been developed from the author's highly successful interdisciplinary course at the University of Rochester attended by science and engineering graduate students.
Review
"In this book [Mukamel] has brought his many contributions together and has woven a fabric that brilliantly ties fundamental principles to experiment with an elegant formalism. This book is of extraordinary value to both the advanced student and researcher in the field. "[It] is written in such a way that it serves as both an advanced text as well as a reference book for the experimentalist. Prof. Mukamel has developed a very powerful unified correlation approach that is applicable to condensed phase systems as well the gas phase. The book provides Green's function techniques which are useful for interpreting nonlinear spectra of frequency and time domain nonlinear spectra of frequency and time domain complex systems. Several applications of current interest are treated in the book including Raman spectrocopies, photon echoes, pump-probe, hole burning, polarization spectroscopies, and impulsive effects.
"Possibly the most important contribution made by this book is that it brings together the techniques of nonlinear spectrosopies with analytical and conceptual foundations that make an important step toward creating a new science for probing the properties of matter."--Charles V. Shank, Director, Lawrence Berkeley National Laboratory
"I can recommend this book wholeheartedly both as a textbook in a graduate course in modern fast spectroscopy and as a reference mongraph for researchers in the field."--Robert J. Silbey, Journal of the American Chemical Society
Table of Contents
1. Introduction
2. Quantum Dynamics in Hilbert Space
3. The Density Operator and Quantum Dynamics in Liouville Space
4. Quantum Electrodynamics, Optical Polarization, and Nonlinear Spectroscopy
5. Nonlinear Response Functions and Optical Susceptibilities
6. The Optical Response Functions of a Multilevel System with Relaxation
7. Semiclassical Simulation of the Optical Response Functions
8. The Cumulant Expansion and the Multimode Brownian Oscillator Model
9. Fluorescence, Spontaneous-Raman and Coherent-Raman Spectroscopy
10. Selective Elimination of Inhomogeneous Broadening; Photon Echoes
11. Resonant Gratings, Pump-Probe, and Hole Burning Spectroscopy
12. Wavepacket Dynamics in Liouville Space; The Wigner Representation
13. Wavepacket Analysis of Nonimpulsive Measurements
14. Off-Resonance Raman Scattering
15. Polarization Spectroscopy; Birefringence and Dichroism
16. Nonlinear Response of Molecular Assemblies; The Local-Field Approximation
17. Many Body and Cooperative Effects in the Nonlinear Response