期刊
JOURNAL OF CHEMICAL PHYSICS
卷 135, 期 11, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3636081
关键词
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资金
- EPSRC
- Imperial College London
- Engineering and Physical Sciences Research Council [EP/E045219/1] Funding Source: researchfish
- EPSRC [EP/E045219/1] Funding Source: UKRI
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, Forster 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. (C) 2011 American Institute of Physics. [doi:10.1063/1.3636081]
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