Principles of Nonlinear Optical SpectroscopyThis 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. |
Contents
Introduction | 3 |
Quantum Dynamics in Hilbert Space | 15 |
Linear Vector Spaces and Operators | 40 |
Copyright | |
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absorption approximation bath Brownian oscillator model calculated Chapter Chem classical cm¯¹ coherent contribution coordinates correlation function coupling defined degrees of freedom denote density operator depends dephasing dipole doorway eigenstates electronic emission equations of motion evolution excited exciton expression factor femtosecond Figure fluorescence four-wave mixing Fourier transform frequency domain given Green function Hamiltonian Hermitian conjugate Hilbert space homogeneous inhomogeneous broadening interaction k₁ limit linear response function lineshape matrix elements mode molecular molecules Mukamel nonlinear optical nonlinear response function nuclear dynamics obtain off-resonant optical response overdamped particle phase space photon photon echo Phys polarization probe propagation pulse pump quantum radiation field Raman relaxation representation represents resonance semiclassical signal spectrum Stokes shift susceptibilities t₁ t₂ techniques time-domain timescale transition two-exciton variables vector vibrational vibronic w₁ w₂ wavefunction wavepacket wavevector Wigner window wavepackets ω₁