Abstract

Fifth-order temporally two-dimensional (2D) Raman scattering probes the structural dynamics in condensed phase systems on a microscopic level. In this experiment a sequence of five non-resonant laser pulses is applied, which probes the two-time correlation function of the polarizability. This quantity is sensitive to the memory time(s) of the local environment and can discriminate between homogeneous and inhomogeneous processes. Therefore, 2D Raman scattering surpasses ordinary one-dimensional Raman techniques such as the optical Kerr effect and transient grating scattering, that measure the total line width but are not sensitive to the line broadening mechanism.

© 1998 IEEE