Picosecond vibrational cooling in mixed molecular crystals studied with a new coherent raman scattering technique

Abstract

We demonstrate the pump-induced coherent Stokes Raman scattering (CSRS) technique by measuring vibrational cooling in low temperature crystals of pentacene in naphthalene following excitation of a vibration 747 cm −1 above the S 1 origin. Using picosecond photon echoes and a two-color pump-probe technique, we find that the initial state decays in 33 ps, and reappears at the origin 25 ps later. We show that pump-induced CSRS simultaneously measures the decay from the initial state and reappearance at the origin. This technique has many of the advantages of conventional coherent Raman (e.g. intense coherent signals), but is a direct measure of the population dynamics in the initial and final states.