Decoherence and quantum interference in a four-site model system: Mechanisms and turnovers

Mahdi Zarea; Daniel Powell; Nicolas Renaud; Michael R. Wasielewski; Mark A. Ratner

doi:10.1021/jp3102942

Decoherence and quantum interference in a four-site model system: Mechanisms and turnovers

Mahdi Zarea^*, Daniel Powell, Nicolas Renaud, Michael R. Wasielewski, Mark A. Ratner

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

We study quantum interference effects in a four-level system which can be used as a minimal model to understand such behavior in systems from synthetic molecular structures to the photosystem-1 reaction center. The effects of environmental decoherence and relaxation on the electron transfer rate are investigated for several types of decoherence processes. The rate as a function of decoherence amplitude shows Kramers turnover, as expected. However, various decoherence processes affect the quantum interference differently. It is shown that when the bridge sites are not dephased the superexchange transfer is enhanced by constructive quantum interference. Dephasing on bridge sites opens a (classical) diffusive channel for fast electron transfer, which can dominate the superexchange current and reduce the constructive quantum interference.

Original language	English (US)
Pages (from-to)	1010-1020
Number of pages	11
Journal	Journal of Physical Chemistry B
Volume	117
Issue number	4
DOIs	https://doi.org/10.1021/jp3102942
State	Published - Jan 31 2013

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Surfaces, Coatings and Films
Materials Chemistry

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title = "Decoherence and quantum interference in a four-site model system: Mechanisms and turnovers",

abstract = "We study quantum interference effects in a four-level system which can be used as a minimal model to understand such behavior in systems from synthetic molecular structures to the photosystem-1 reaction center. The effects of environmental decoherence and relaxation on the electron transfer rate are investigated for several types of decoherence processes. The rate as a function of decoherence amplitude shows Kramers turnover, as expected. However, various decoherence processes affect the quantum interference differently. It is shown that when the bridge sites are not dephased the superexchange transfer is enhanced by constructive quantum interference. Dephasing on bridge sites opens a (classical) diffusive channel for fast electron transfer, which can dominate the superexchange current and reduce the constructive quantum interference.",

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T1 - Decoherence and quantum interference in a four-site model system

T2 - Mechanisms and turnovers

AU - Zarea, Mahdi

AU - Powell, Daniel

AU - Renaud, Nicolas

AU - Wasielewski, Michael R.

AU - Ratner, Mark A.

PY - 2013/1/31

Y1 - 2013/1/31

N2 - We study quantum interference effects in a four-level system which can be used as a minimal model to understand such behavior in systems from synthetic molecular structures to the photosystem-1 reaction center. The effects of environmental decoherence and relaxation on the electron transfer rate are investigated for several types of decoherence processes. The rate as a function of decoherence amplitude shows Kramers turnover, as expected. However, various decoherence processes affect the quantum interference differently. It is shown that when the bridge sites are not dephased the superexchange transfer is enhanced by constructive quantum interference. Dephasing on bridge sites opens a (classical) diffusive channel for fast electron transfer, which can dominate the superexchange current and reduce the constructive quantum interference.

AB - We study quantum interference effects in a four-level system which can be used as a minimal model to understand such behavior in systems from synthetic molecular structures to the photosystem-1 reaction center. The effects of environmental decoherence and relaxation on the electron transfer rate are investigated for several types of decoherence processes. The rate as a function of decoherence amplitude shows Kramers turnover, as expected. However, various decoherence processes affect the quantum interference differently. It is shown that when the bridge sites are not dephased the superexchange transfer is enhanced by constructive quantum interference. Dephasing on bridge sites opens a (classical) diffusive channel for fast electron transfer, which can dominate the superexchange current and reduce the constructive quantum interference.

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Decoherence and quantum interference in a four-site model system: Mechanisms and turnovers

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