A. Tokmakoff et al., THE INTERMOLECULAR INTERACTION MECHANISMS IN LIQUID CS2 AT 295 AND 165 K PROBED WITH 2-DIMENSIONAL RAMAN-SPECTROSCOPY, Chemical physics, 233(2-3), 1998, pp. 231-242
Two-dimensional Raman spectroscopy is used to probe the intermolecular
interaction dynamics of CS2 at 295 and 165 K. The influence of nonlin
ear polarizability and liquid anharmonicity on the observable is discu
ssed. It is found that the response at both temperatures is dominated
by the nonlinear polarizability, which is most likely due to interacti
on-induced effects. A model using three Brownian oscillators to repres
ent the collective motions on three time scales is unable to reproduce
the 295 K data. At low temperature, the model presumably works better
as a result of the time-scale separation between the inertial and dif
fusive dynamics. (C) 1998 Elsevier Science B.V. All rights reserved.