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1 2009

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Nonradiative electron and energy transfer. Explicit estimation of the influence of coherent and dephasing processes in a vibrational bath on electronic dynamics

Menšík M., Král L.

Materials Science Poland

2009

Vol. 27, No. 3

671--684

A theoretical model is studied of the coupling of several electronic states to a vibrational manifold. In this approach, the vibrational manifold is divided into two subbaths. The first one, a coherent subbath, interacts coherently with electronic states. The second one, a thermalizing subbath, is responsible for relaxation of vibronic energy. In the first step, the thermalizing subbath is projected out, under the assumption of a standard (Markovian) approximation in the interaction picture and the effective dissipative Liouville equation for a coherent vibronic system (electronic states + coherent bath modes) is thus obtained. Next, "coherent bath modes" are also projected out and irreversible master equations for electronic degrees of freedom are obtained, even without the Markovian approximation. Analytical expressions based on the double projection technique are compared with numerical simulations of a two-level electronic systems interacting with a single vibrational mode embedded in the dissipative environment. We show that the double projection technique can be applied to predict spikes of resonant amplification of electron (vibronic) energy transfer, as well as to analytically test various models of kinetic theories.