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

Fei Ma*, Elisabet Romero, Michael R. Jones, Vladimir I. Novoderezhkin, Rienk van Grondelle

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review

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.

Original languageEnglish
Article number933
Pages (from-to)1-9
Number of pages9
JournalNature Communications
Volume10
DOIs
Publication statusPublished - 25 Feb 2019

Funding

F.M., E.R. and R.v.G. were supported by an Advanced Investigator grant from the European Research Council (No. 267333, PHOTPROT) to R.v.G. and the TOP-grant (700.58.305) from the Foundation of Chemical Science part of NWO. R.v.G. gratefully acknowledges his Academy Professor grant from the Netherlands Royal Academy of Sciences (KNAW). M.R.J. acknowledges support from the Biotechnology and Biological Sciences Research Council of the UK (project BB/I022570/1). V.I.N. was supported by the Russian Foundation for Basic Research (Grant No. 18-04-00105).

FundersFunder number
Foundation of Chemical Science
Netherlands Royal Academy of Sciences
Seventh Framework Programme267333
Biotechnology and Biological Sciences Research CouncilBB/I022570/1
European Research Council700.58.305
Koninklijke Nederlandse Akademie van Wetenschappen
Russian Foundation for Basic Research18-04-00105
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

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