Two-dimensional Raman spectroscopy of vibrational interactions in liquids

Two-dimensional fifth-order Raman spectroscopy has the ability to probe nonlinear interactions between well defined vibrational motions in liquids. It can reveal the nonlinear dependence of the molecular polarizability on vibrational coordinates, intermolecular interaction-induced effects, and anharmonic couplings between modes. We use this technique to probe these interactions at an intramolecular level in liquid CCl4 and CHCl3, and at an intermolecular level in a mixture of these two liquids.