Perturbative treatment of intercenter coupling in Redfield theory

Details Perturbative treatment of intercenter coupling in Redfield theory Perturbative treatment of intercenter coupling in Redfield theory

2000-12-06

arxiv.org/abs/physics/0012012v1

Chem. Phys. 268, 121-130 (2001)

Physics

Chemical Physics

Scientific paper

10.1016/S0301-0104(01)00288-9

The quantum dynamics of coupled subsystems connected to a thermal bath is studied. In some of the earlier work the effect of intercenter coupling on the dissipative part was neglected. This is equivalent to a zeroth-order perturbative expansion of the damping term with respect to the intercenter coupling. It is shown numerically for two coupled harmonic oscillators that this treatment can lead to artifacts and a completely wrong description, for example, of a charge transfer processes even for very weak intercenter coupling. Here we perform a first-order treatment and show that these artifacts disappear. In addition, we demonstrate that the thermodynamic equilibrium population is almost reached even for strong intercenter coupling strength.

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