Principles of Nonlinear Optical Spectroscopy

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.

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

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 "Professor Mukamel, a well known and accomplished theoretical physical chemist, has written an up-to-date and comprehensive monograph/textbook on nonlinear optical spectroscopy. Although the focus is theoretical, the attention paid to describing modern experiments is noteworthy. This book is unusual in its completeness: the theoretical development assumes only a standard quantum mechanics course, but goes all the way to the most recent developments; the attention to experiments and what can be learned about molecular dynamics from them is as deep and definitive as the theory. I can recommend this book wholeheartedly both as a textbook in a graduate course in modern fast spectroscopy, and as a reference monograph for researchers in the field."--Robert J. Sibley, MIT, in the Journal of the American Chemical Society "Mukamel has developed a powerful and intuitively satisfying description of dynamical nonlinear spectroscopy which allows the enormous variety of nonlinear spectroscopies to be described and analyzed on a common footing. A student who has mastered graduate quantum mechanics should be able to cope with this material. This book is likely to be essential reading for workers in a wide variety of fields impinging on the dynamics of complex, condensed phase systems. The book will be important both for the design of new experiments as well as their analysis. Mukamel is to be congratulated on this superb book, and his publisher deserves credit for keeping the price within the reach of graduate students and their professors."--Graham R. Fleming, University of California, Berkeley, and Director, Physical Biosciences Division, Lawrence Berkeley National Laboratory "This book is mandatory for workers at the frontier of condensed phase nonlinear spectroscopy. The author is uniquely capable of putting this material together. The book is clearly a work of love. It is complete, deep, and authoritative. The writing has the clarity and coherence expected for a single-author work."--John C. Wright, University of Wisconsin, in Analytical Chemistry "The book is well-organized and contains many references and an extensive index. It is ideal for graduate and post-doctorate students. It is also invaluable for senior staff wishing to become educated on the theoretical state-of-the-art in this field. Stimulated by the recent developments in ultrafast laser technology, progress in the field of nonlinear optical spectroscopy occurs at an increasing pace. Because of Mukamels book there is hope that scientists worldwide will speak a common language, easing communication and stimulating cooperation." --Douwe A. Wiersma, University of Groningen, in Optics and Photonics News * This review takes up two fields (too long to fit into one) "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 "An excellent account of the application of modern Liouville space methods to the theory of nonlinear optical spectroscopy by a pioneer of this approach."--Marvin D. Girardeau, University of Oregon