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Vibronic Coherence in the Charge Separation Process of the Rhodobacter sphaeroides Reaction Center

Research output: Contribution to journalLetter

  • Fei Ma
  • Elisabet Romero
  • Michael R. Jones
  • Vladimir I. Novoderezhkin
  • Rienk Van Grondelle
Original languageEnglish
Pages (from-to)1827-1832
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume9
Issue number8
Early online date27 Mar 2018
DOIs
DateAccepted/In press - 27 Mar 2018
DateE-pub ahead of print - 27 Mar 2018
DatePublished (current) - 19 Apr 2018

Abstract

Two-dimensional electronic spectroscopy was applied to a variant of the reaction center (RC) of purple bacterium Rhodobacter sphaeroides lacking the primary acceptor ubiquinone in order to understand the ultrafast separation and transfer of charge between the bacteriochlorin cofactors. For the first time, characteristic 2D spectra were obtained for the participating excited and charge-transfer states, and the electron-transfer cascade (including two different channels, the P∗ and B∗ channels) was fully mapped. By analyzing quantum beats using 2D frequency maps, excited-state vibrational modes at 153 and 33 cm-1 were identified. We speculate that these modes couple to the charge separation (CS) process and collectively optimize the CS and are responsible for the superhigh efficiency.

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  • Full-text PDF (accepted author manuscript)

    Rights statement: This is the author accepted manuscript (AAM). The final published version (version of record) is available online via ACS at https://pubs.acs.org/doi/10.1021/acs.jpclett.8b00108. Please refer to any applicable terms of use of the publisher.

    Accepted author manuscript, 1 MB, PDF document

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