Tic. Jansen et al., Interaction induced effects in the nonlinear Raman response of liquid CS2:A finite field nonequilibrium molecular dynamics approach, J CHEM PHYS, 114(24), 2001, pp. 10910-10921
The third- and fifth-order time-domain Raman responses of liquid carbon dis
ulfide have been calculated, taking local field effects into account throug
h the dipole-induced dipole approximation to the polarizability. The third-
order response is shown to be in excellent agreement with experimental data
. The calculated two-dimensional shape of the fifth-order response is compa
red with recently reported experimental observations of what is claimed to
be pure fifth-order response. Considerable discrepancies are observed which
might be explained by contamination of the experimental results with seque
ntial and especially parallel third-order cascaded Raman response. A new ch
oice of polarization conditions is proposed, which increases the discrimina
tion against these unwanted cascading effects, as compared to the previousl
y discussed fully polarized and magic angle conditions. (C) 2001 American I
nstitute of Physics.