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

Abstract

In this paper we report the measurement of the direct fifth-order electronically nonresonant intermolecular response from liquid ${\mathrm{CS}}_{\mathrm{2}}$ 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 ${\mathrm{CS}}_{\mathrm{2}}$ at room temperature is well described as homogenous. Comparisons of the data to simulations are discussed.