Abstract
It is demonstrated how time-frequency resolved coherent Raman scattering (CRS) signals generated by broadband, non-transform limited, quasi-cw (noisy) light can be sensitive probes of molecular vibrational dynamics. The coherent Raman scattering signals from molecular liquids and their mixtures with noisy light are dispersed onto a CCD array and probed interferometrically to produce time-frequency domain spectrograms. These spectrograms offer an extensive oversampling of the data resulting in improved precision of measured parameters over previous noisy light methods. This technique has been very useful in measuring small changes in material parameters, such as Raman frequency shifts and linewidth changes, in dilution series with Raman inactive diluents. Very recently theory and experiment have extended to include mixtures with multiple Raman resonances. Several examples of experiments are presented and discussed.