The third- and fifth-order nonlinear Raman response of liquid CS2 calculated using a finite field nonequilibrium molecular dynamics method

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. (C) 2000 American Institute of Physics. [S0021-9606(00)50223-2].