Ultrafast nonlinear spectroscopy with chirped optical pulses

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Abstract
Ultrafast four-wave mixing experiments using chirped-pulse excitation of a dye molecule in solution are reported and analyzed. Novel time-delayed signals are observed which are assigned to coherent Stokes-Raman scattering involving the excited state. Numerical calculations of four-wave mixing with linearly chirped pulses based on a stochastic dynamical model show that the signal near zero delay time is extremely sensitive to the presence or absence of slow fluctuations in the solute-solvent interaction.