Physics – Quantum Physics
Scientific paper
2011-07-04
J. Chem. Phys. 135, 114501 (2011)
Physics
Quantum Physics
13 pages, 6 figures, comments welcome. Published version, minor changes to text, references added
Scientific paper
10.1063/1.3636081
We investigate the energy transfer dynamics in a donor-acceptor model by developing a time-local master equation technique based on a variational transformation of the underlying Hamiltonian. The variational transformation allows a minimisation of the Hamiltonian perturbation term dependent on the system parameters, and consequently results in a versatile master equation valid over a range of system-bath coupling strengths, temperatures, and environmental spectral densities. While our formalism reduces to the well-known Redfield, Foerster and polaron forms in the appropriate limits, in general it is not equivalent to perturbing in either the system-environment or donor-acceptor coupling strengths, and hence can provide reliable results between these limits as well. Moreover, we show how to include the effects of both environmental correlations and non-equilibrium preparations within the formalism.
McCutcheon Dara P. S.
Nazir Ahsan
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