Non-Linear Optical Spectroscopy and Molecular Dynamics in Liquids

Abstract

Selected for discussion in this paper are some recent studies we have undertaken to investigate nonlinear optical spectroscopy, in both the time and frequency domain, as a tool for exploring molecular liquids and binary systems. . The issues we address are important to both the development of a microscopic picture of molecular dynamics and the influence of those motions of the dynamics of photophysical and photochemical processes, as well as on chemical reaction which take place from the ground electronic states. In some respects, given our long standing research interests on the picosecond dynamics of electron solvation, one might subtitle this paper “solvation revisited”, since an underlying theme of this work is the nature of solvation dynamics and solvation structures in chemical systems. Ultrashort laser pulses(l) now offer direct access to the picosecond (ps) and femtosecond (fs) time domain. What are some of the challenges that we meet at this frontier?