2-DIMENSIONAL RAMAN-SPECTROSCOPY OF VIBRATIONAL INTERACTIONS IN LIQUIDS

Two-dimensional fifth-order Raman spectroscopy has the ability to prob e nonlinear interactions between well defined vibrational motions in l iquids. It can reveal the nonlinear dependence of the molecular polari zability on vibrational coordinates, intermolecular interaction-induce d effects, and anharmonic couplings between modes. We use this techniq ue to probe these interactions at an intramolecular level in liquid CC l4 and CHCl3, and at an intermolecular level in a mixture of these two liquids.