Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 114, Issue 48, Pages 20362-20369Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp103369s
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Funding
- Belgian Federal Government
- UCSD
- U.S.-Israel Binational Science Foundation
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We propose a self-consistent generalized quantum master equation (GQME) to describe electron transport through molecular junctions. In a previous study [Esposito, M.; Galperin, M. Phys. Rev, B 2009, 79, 205303], we derived a time-nonlocal GQME to cure the lack of broadening effects in Redfield theory. To do so, the free evolution used in the Born-Markov approximation to close the Redfield equation was replaced by a standard Redfield evolution. In the present paper, we propose a backward Redfield evolution leading to a time-local GQME which allows for a self-consistent procedure of the GQME generator. This approach is approximate but properly reproduces the nonequilibrium steady-state density matrix and the currents of an exactly solvable model. The approach is less accurate for higher moments such as the noise.
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