A finite field molecular dynamics (MD) method has been developed to calculate the off-resonant Raman response of liquids. The method has been used to calculate the third- and fifth-order optical responses of CS2. From the third-order response, the intensity of third-order cascading processes has been estimated. The calculated ratio between the fifth-order intensity and the intensity of the third-order cascading processes supports experimental observations, claiming that two-dimensional Raman spectra are dominated by third-order cascading processes. © 2000 American Institute of Physics.

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