From Fundamental Theories to Quantum Coherences in Electron Transfer

Shahnawaz Rafiq, Gregory D. Scholes

Research output: Contribution to journalReview articlepeer-review

81 Scopus citations


Photoinduced electron transfer (ET) is a cornerstone of energy transduction from light to chemistry. The past decade has seen tremendous advances in the possible role of quantum coherent effects in the light-initiated energy and ET processes in chemical, biological, and materials systems. The prevalence of such coherence effects holds a promise to increase the efficiency and robustness of transport even in the face of energetic or structural disorder. A primary motive of this Perspective is to work out how to think about "coherence" in ET reactions. We will discuss how the interplay of basic parameters governing ET reactions - like electronic coupling, interactions with the environment, and intramolecular high-frequency quantum vibrations - impact coherences. This includes revisiting the insights from the seminal work on the theory of ET and time-resolved measurements on coherent dynamics to explore the role of coherences in ET reactions. We conclude by suggesting that in addition to optical spectroscopies, validating the functional role of coherences would require simultaneous mapping of correlated electron motion and atomically resolved nuclear structure.

Original languageEnglish
Pages (from-to)708-722
Number of pages15
JournalJournal of the American Chemical Society
Issue number2
StatePublished - Jan 16 2019

Bibliographical note

Funding Information:
S.R. and G.D.S. acknowledge support from the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, of the U.S. Department of Energy through Grant No. DE-SC0015429.

Publisher Copyright:
Copyright © 2018 American Chemical Society.

ASJC Scopus subject areas

  • Catalysis
  • Chemistry (all)
  • Biochemistry
  • Colloid and Surface Chemistry


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