Direct fifth-order electronically nonresonant Raman scattering from CS2 atroom temperature

In this paper we report the measurement of the direct fifth-order electroni cally nonresonant intermolecular response from liquid CS2 at room temperatu re. We recently demonstrated that all previous attempts to measure the dire ct fifth-order response were dominated by third-order cascaded signals [J. Chem Phys. 111, 3105 (1999)]. Here we show that phase matching consideratio ns can be used to provide substantial discrimination against the cascaded t hird-order signals, and the direct fifth-order response can be measured. Th e measured responses indicate that the intermolecular spectrum of liquid CS 2 at room temperature is well described as homogenous. Comparisons of the d ata to simulations are discussed. (C) 2000 American Institute of Physics. [ S0021-9606(00)00625-5].