Table of Contents
Laser Chemistry
Volume 19 (1999), Issue 1-4, Pages 91-96

Temporally Two-Dimensional Fifth-Order Raman Scattering on Intermolecular Vibrations in Cs2/Pentane Binary Mixtures

1Ultrafast Laser and Spectroscopy Laboratory, Dept. of Chemical Physics, Mat. Science Center, University of Groningen, Groningen 9747 AG, The Netherlands
2Dept. of Chemistry, Osaka University, Toyonaka 560, Japan

Received 7 April 1997

Copyright © 1999 Hindawi Publishing Corporation. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.


Third- and fifth-order impulsive stimulated Raman scattering experiments are performed to study low-frequency intermolecular vibrations in CS2/pentane binary mixtures. The changes of the optical Kerr effect response cannot be assigned unequivocally to a single microscopic process. In particular, the homogeneous and inhomogeneous line broadening mechanisms cannot be determined. Temporally two-dimensional Raman scattering experiments indicate that the correlation time of fluctuations of the intermolecular potential decreases upon dilution. The experimental results give evidence of strong coupling between the ultrafast coherent vibrations and the slow reorientational diffusion.