Articles you may be interested inFifth-order two-dimensional Raman spectroscopy of liquid water, crystalline ice Ih and amorphous ices: Sensitivity to anharmonic dynamics and local hydrogen bond network structure Interaction induced effects in the nonlinear Raman response of liquid CS 2 : A finite field nonequilibrium molecular dynamics approach A finite field molecular dynamics ͑MD͒ 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 CS 2 . 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.