Interferometric Down-Conversion of High-Frequency Molecular Vibrations with Time−Frequency-Resolved Coherent Raman Scattering Using Quasi-CW Noisy Light: C−H Stretching Modes of Chloroform and Benzene

Abstract

For the first time, the high-frequency symmetric C−H stretching modes of chloroform and benzene are down-converted using the recently developed time−frequency-resolved interferometric coherent anti-Stokes Raman scattering with broad-band nontransform limited (noisy) light excitation method. As an application, chloroform−carbon tetrachloride, benzene−benzene-d6 and benzene−acetone-d6 dilution series are performed. Concentration-dependent Raman frequencies and vibrational dephasing rate constants are observed by this new technique.