Direct fifth-order electronically nonresonant Raman scattering from CS2 at room temperature

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