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 calcula te 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 thi rd-order response, the intensity of third-order cascading processes has bee n estimated. The calculated ratio between the fifth-order intensity and the intensity of the third-order cascading processes supports experimental obs ervations, claiming that two-dimensional Raman spectra are dominated by thi rd-order cascading processes. (C) 2000 American Institute of Physics. [S002 1-9606(00)50223-2].