Response function theory of time-resolved CARS and CSRS of rotating molecules in liquids under general polarization conditions

Abstract

A theoretical treatment of time-resolved CARS and CSRS is given that includes molecular rotation during the time interval between the excitation and probing light pulses. A molecular response function tensor is found that accounts for the vibrational relaxation and the rotational diffusion of the molecules. The ensemble average of this response function with an arbitrary set of polarization conditions for the light pulses yields a sum of three terms. Each term is the product of a polarization factor P l and a molecular rotational relaxation function M l . New polarization conditions are proposed that permit to measure each of these three terms separately.