TY - JOUR
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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U2 - 10.1021/jp3102942
DO - 10.1021/jp3102942
M3 - Article
C2 - 23286386
AN - SCOPUS:84874450127
SN - 1520-6106
VL - 117
SP - 1010
EP - 1020
JO - Journal of Physical Chemistry B
JF - Journal of Physical Chemistry B
IS - 4
ER -