Temporally two-dimensional overtone vibrational dephasing spectroscopy in liquids

A temporally two-dimensional overtone vibrational dephasing spectroscopy, which is based on the fifth-order nonlinearity, is proposed to investigate correlation between fluctuations of different vibrational frequencies in liquids. The experiment is done for the C-D stretching of neat CDCl3 liquid. We found that a signal decay as a function of the second-pulse interval gets faster as the first-pulse interval increases.