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.
Highlights
Coherent Raman scattering (CRS) has long been a useful probe of condensed phase dynamics providing information on Raman frequencies, line widths (’YR) and hyperpolarizabilities. ’Conventional’coherent Raman scattering (CRS) is a frequency domain technique in which the signal intensity is measured as a function of the frequency difference between two narrowband laser sources
CRS is a frequency domain technique in which the signal intensity is measured as a function of the frequency difference between two narrowband laser sources
[1 ], it was discovered that broadband, non-transform limited, quasi-cw light sources could provide interferometric time resolution that is governed by the correlation time of the noisy light, and not by the temporal profile of the pulse which is typically nanoseconds long
Summary
CRS is a frequency domain technique in which the signal intensity is measured as a function of the frequency difference between two narrowband laser sources. Is the instrument response correction consisting of a nonzero slitwidth of the monochromator and a nonzero bandwidth of the narrowband beam, (ii) the noisy field frequencies are completely absent and (iii) for fixed cot and COR, A depends only on the position in frequency space at which the signal is detected (az) and represents a strong down-conversion of the Raman mode (when CaD CaM + 2CaR).
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