THE INFLUENCE OF HIGH-FREQUENCY MODES ON 2 PULSE SPECTROSCOPY

Theoretical analyses of molecular response to ultrafast pulse excitati on often do not account for the influence of high frequency modes on t he spectrum of the molecule. In a previous article [M. N. Kobrak, E. M . Hiller, and S. A. Rice, J. Chem. Phys. 105, 9403 (1996)], we have sh own that the high frequency modes of the molecule can dramatically cha nge the distribution of an observable in processes initiated by a sing le ultrashort pulse. In this article we extend our treatment to allow for two-pulse processes, and apply the results to two models which hav e a qualitative resemblence to bacteriorhodopsin. (C) 1997 American In stitute of Physics.