Time resolved direct probing of the change in the local solvent response following excitation of a solute

The change in the low frequency (0.1 - 500 cm^-1) non-resonant Raman response following excitation of a dye molecule in solution has been measured as a function of time after resonant excitation of a solute using a two-dimensional mixed resonant, non-resonant time domain spectroscopy. This method provides a direct measurement of the change in the spectrum of the local environment as a dynamic event proceeds in a condensed phase.