title: Fifth-order raman spectrum of an atomic liquid: simulation and instantaneous-normal-mode calculation
abstract: Experimental artifacts and technical difficulties in carrying out theoretical calculations have consistently frustrated attempts to obtain the two-dimensional (5th-order) Raman spectrum of a liquid. We report here a new theoretical development: the first microscopic numerical simulation of the 5th-order Raman signal in a liquid. Comparison with an instantaneous-normal-mode treatment, a fully microscopic model which interprets liquid dynamics as arising from coherent harmonic modes, shows that the 5th-order spectrum reveals profound effects stemming from dynamical anharmonicity.
authors.affiliation: Department of Chemistry, Brown University, Providence, Rhode Island 02912, USA.
authors.initials: A
authors.lastname: Ma
authors.initials: RM
authors.lastname: Stratt