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Heterodyne-detected fifth-order nonresonant Raman scattering from room temperature CS2.

Actively phase-locked heterodyne-detected fifth-order nonresonant Raman scattering from room temperature CS2 has been measured. The experimental signals have similar magnitudes, shapes, and sign changes as calculated responses obtained via molecular dynamics simulations [S. Saito and I. Ohmine, Phys. Rev. Lett. 88, 207401 (2002)]. The measured signals contain sign changes that appear to be associated with the coupling of rotational motions both to each other and to translational motions.