Coherent nuclear motion in a condensed-phase environment: Wave-packet approach and pump-probe spectroscopy

Details Coherent nuclear motion in a condensed-phase environment: Wave-packet approach and pump-probe spectroscopy Coherent nuclear motion in a condensed-phase environment: Wave-packet approach and pump-probe spectroscopy

1999-01-13

arxiv.org/abs/physics/9901015v1

J.Chem.Phys. 110, 5851 (1999)

Physics

Chemical Physics

12 page, 13 figures

Scientific paper

10.1063/1.478484

A quantum-mechanical Gaussian wave-packet approach to the theoretical description of nuclear motions in a condensed-phase environment is developed. General expressions for the time-dependent reduced density matrix are given for a harmonic potential surface, and the exact quantum dynamics is found for a microscopic system-plus-bath model. Particular attention is devoted to the influence of initial correlations between system and bath for the outcome of a pump-probe experiment. We show that the standard factorized preparation, compared to a more realistic correlated preparation, leads to significantly different stimulated emission spectra at high temperatures. Recent experiments for the reaction center are analyzed using this formalism.

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