Unified description of electron transfer and nonlinear optical spectroscopy

Abstract

Recent developments in nonlinear optical spectroscopy, in particular the successful application of femtosecond laser pulses, provide a direct probe for elementary photophysical and photochemical processes. The dynamics and relaxation processes in semiconductors, solvated dye molecules, elementary reaction events, and the solvated electron were monitored with remarkable temporal and spectral resolution. In this Account the authors present a semiclassical theoretical framework that provides a unified description of molecular rate processes and nonlinear optical spectroscopy.