Electron transfer in multiply bridged donor-acceptor molecules

Dephasing and quantum coherence

Randall H. Goldsmith, Michael R Wasielewski, Mark A Ratner

Research output: Contribution to journalArticle

50 Citations (Scopus)

Abstract

We present a simple theoretical treatment of nonadiabatic electron transfer in multiply bridged donor-bridge-acceptor molecules using the density matrix formalism. Destructive interference can result from different signed couplings between bridge sites, with the simplest system being a four-site Joachim-type molecular interferometer. Previous work has shown that deposition of energy on the bridge sites erases the interference and recovers transport. We show that pure local dephasing, a completely elastic process, is also capable of eliminating destructive interference and regaining transport. Destructive interference as a result of system connectivity can explain the familiar ortho-meta-para reactivity of benzene bridges. We also show that pure dephasing can yield a coalescence of ortho, meta, and para effective coupling strengths and suggest a system to observe this effect experimentally.

Original languageEnglish
Pages (from-to)20258-20262
Number of pages5
JournalJournal of Physical Chemistry B
Volume110
Issue number41
DOIs
Publication statusPublished - Oct 19 2006

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electron transfer
interference
Molecules
Electrons
molecules
Benzene
Coalescence
Interferometers
coalescing
interferometers
reactivity
benzene
formalism
energy

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Electron transfer in multiply bridged donor-acceptor molecules : Dephasing and quantum coherence. / Goldsmith, Randall H.; Wasielewski, Michael R; Ratner, Mark A.

In: Journal of Physical Chemistry B, Vol. 110, No. 41, 19.10.2006, p. 20258-20262.

Research output: Contribution to journalArticle

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