Intermolecular spectral densities of liquids: A quantitative comparison of time-domain and frequency-domain techniques

Intermolecular spectral densities measured by two independent experimental techniques, time-domain optical-heterodyne-detected Raman-induced-Kerr-effect spectroscopy (OHD-RIKES) and frequency-domain stimulated gain spectroscopy (SGS), for three molecular liquids (benzene, carbon disulfide, and chloroform) are compared. The agreement in the high-frequency (interaction-induced) portion of the spectrum (20–150 cm−1) is quantitative. The relative merits between time-domain and frequency-domain coherent light-scattering techniques are discussed.