Abstract

Dephasing effects on the ultrafast transient hole-burning spectrum of a nonpolar solute and solvent molecular system are theoretically studied on the basis of an indirect dephasing model. The relative intensity of the transient hole-burning spectrum derived is characterized by a Lorentzian function with peak shift and width broadening which have, respectively, linear and quadratic time-dependence. The peak shift and width broadening are expressed in terms of two parameters, IVR (intramolecular vibrational energy redistribution) rate and the energy difference between the electronic transition before and after the IVR. A qualitative explanation is given for the experimental results of transient hole-burning on nonpolar solute dimethyl- s-tetrazine in viscous solvents reported by Yu, Kang and Berg.

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