Is back-electron transfer process in Betaine-30 coherent?

Shahnawaz Rafiq, Gregory D. Scholes

Research output: Contribution to journalArticle

4 Scopus citations

Abstract

The possible role of coherent vibrational motion in ultrafast photo-induced electron transfer remains unclear despite considerable experimental and theoretical advances. We revisited this problem by tracking the back-electron transfer (bET) process in Betaine-30 with broadband pump-probe spectroscopy. Dephasing time constant of certain high-frequency vibrations as a function of solvent shows a trend similar to the ET rates. In the purview of Bixon-Jortner model, high-frequency quantum vibrations bridge the reactant-product energy gap by providing activationless vibronic channels. Such interaction reduces the effective coupling significantly and thereby the coherence effects are eliminated due to energy gap fluctuations, making the back-electron transfer incoherent.

Original languageEnglish (US)
Pages (from-to)500-506
Number of pages7
JournalChemical Physics Letters
Volume683
DOIs
StatePublished - Sep 1 2017

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Keywords

  • Bixon-Jortner model
  • Coherent dynamics
  • Electron transfer
  • High frequency quantum vibrations
  • Incoherent transfer
  • Marcus inverted region

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