Time-Frequency Resolved Coherent Raman Scattering From Molecular Liquids and Their Mixtures With Quasi-Cw Noisy Light: I(2) CRS Spectrograms

It is demonstrated how time-frequency resolved coherent Raman scattering (CRS)signals generated by broadband, non-transform limited, quasi-cw (noisy) light can besensitive probes of molecular vibrational dynamics. The coherent Raman scatteringsignals from molecular liquids and their mixtures with noisy light are dispersed onto aCCD array and probed interferometrically to produce time-frequency domain spectrograms. These spectrograms offer an extensive oversampling of the data resulting inimproved precision of measured parameters over previous noisy light methods. Thistechnique has been very useful in measuring small changes in material parameters, suchas Raman frequency shifts and linewidth changes, in dilution series with Raman inactivediluents. Very recently theory and experiment have extended to include mixtures withmultiple Raman resonances. Several examples of experiments are presented anddiscussed.