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Both electronic and vibrational coherences are involved in primary electron transfer in bacterial reaction center

Research output: Contribution to journalArticle

  • Fei Ma
  • Elisabet Romero
  • Michael R Jones
  • Vladimir I. Novoderezhkin
  • Rienk van Grondelle
Original languageEnglish
Article number933
Number of pages12
JournalNature Communications
Volume10
DOIs
DateAccepted/In press - 15 Jan 2019
DatePublished (current) - 25 Feb 2019

Abstract

Understanding the mechanism behind the near-unity efficiency of primary electron transfer in reaction centers is essential for designing performance-enhanced artificial solar conversion systems to fulfill mankind’s growing demands for energy. One of the most important challenges is distinguishing electronic and vibrational coherence and establishing their respective roles during charge separation. In this work we apply two-dimensional electronic spectroscopy to three structurally-modified reaction centers from the purple bacterium Rhodobacter sphaeroides with different primary electron transfer rates. By comparing dynamics and quantum beats, we reveal that an electronic coherence with dephasing lifetime of ~190 fs connects the initial excited state, P*, and the charge-transfer intermediate PA+PB-; this P*→PA+PB- step is associated with a long-lived quasi-resonant vibrational coherence; and another vibrational coherence is associated with stabilizing the primary photoproduct, P+BA-. The results show that both electronic and vibrational coherences are involved in primary electron transfer process and they correlate with the super-high efficiency.

    Research areas

  • electron transfer, Reaction kinetics and dynamics, Optical spectroscopy

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    Rights statement: This is the final published version of the article (version of record). It first appeared online via Springer NAture at https://www.nature.com/articles/s41467-019-08751-8#article-info. Please refer to any applicable terms of use of the publisher.

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    Licence: CC BY

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