Raman fringe decay: properties of a four-wave mixing experiment with incoherent light

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Abstract
The results of Raman fringe decay experiments—a four-wave mixing type of experiment that uses incoherent light—on the 524-cm−1 mode of liquid methyl iodide and the 656-cm−1 mode of liquid carbon disulfide are presented for two polarization configurations, yielding significantly different time-dependent behavior. We show that, because it uses incoherent light, the Raman fringe decay is a powerful technique for measuring ultrafast vibrational dephasing. Pronounced detuning oscillations are observed for off-resonant excitation. The theoretical description of the experiments reproduces all the features of the experimental data.