INTERFEROMETRIC COHERENT RAMAN-SPECTROSCOPY WITH INCOHERENT-LIGHT - SOME APPLICATIONS

The theory of Interferometric Coherent Raman Scattering (ICRS) using ''twin'' broadband fields has recently been extended to include both resonant and nonresonant contributions to the signal. It is reviewed here. Valid for both ICARS and ICSRS, it is applied to new ICARS experiments on neat toluene and on alcoholic solutions of a methine dye. In each case the damped Rabi Detuning Oscillations (RDO), that are characteristic of ICRS, lead directly to vibrational frequencies and their dephasing times. The theory is also applied as a new way to determine the ratio of the nonresonant to resonant hyperpolarizabilities, accurately for toluene, and approximately for the methine dye solution whose (vibrationally) ''nonresonant'' contribution is negative.