Polarization Effects of Time-Resolved Coherent Raman Scattering in Liquids

Abstract

Ultrafast excitation and subsequent probing of molecular vibrations in liquids and gases and of lattice vibrations in solids have received increasing interest in recent years /1,2/. Using coherent Raman scattering of delayed probing pulses after stimulated Raman excitation, the dephasing of molecular vibrations or of lattice modes was directly studied. Most of the previous work has been performed under special polarization conditions with parallel polarization for the excitation and the probing process. The present paper is devoted to more general studies in the liquid case. Theoretical and experimental data will be presented, demonstrating that the observed signal transients and the obtained information are vastly different, depending on the specific polarization conditions.