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

Research output: Contribution to journalArticlepeer-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 languageEnglish (US)
Pages (from-to)1010-1020
Number of pages11
JournalJournal of Physical Chemistry B
Volume117
Issue number4
DOIs
StatePublished - Jan 31 2013

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

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