LIQUID DYNAMICS STUDIED BY HIGHER-ORDER NONLINEAR-OPTICAL SPECTROSCOPY

Temporally two-dimensional non-resonant Raman spectroscopies, which ar e based on higher order susceptibilities, have been developed to disti nguish homogeneous and inhomogeneous contributions to vibrational deph asing. The five-pulse correlation experiment was performed to study lo w frequency intermolecular vibrational dephasing of liquid CS2, and th e Raman echo experiment was conducted to investigate the C=N stretchin g of benzonitrile. In the both cases it is found that homogeneous deph asing is dominant.