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

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

doi:10.1021/acs.jpclett.8b00108

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

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

^*Corresponding author for this work

Research output: Contribution to Journal › Article › Academic › peer-review

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.

Original language	English
Pages (from-to)	1827-1832
Number of pages	6
Journal	Journal of Physical Chemistry Letters
Volume	9
Issue number	8
Early online date	27 Mar 2018
DOIs	https://doi.org/10.1021/acs.jpclett.8b00108
Publication status	Published - Apr 2018

Funding

F.M., E.R., and R.v.G. were supported by an Advanced Investigator grant from the European Research Council (No. 267333, PHOTPROT) 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 U.K. (Project BB/I022570/ 1).

Funders	Funder number
Netherlands Royal Academy of Sciences
Seventh Framework Programme
Foundation of Chemical Science
Koninklijke Nederlandse Akademie van Wetenschappen
UK Research and Innovation
European Commission	267333
Biotechnology and Biological Sciences Research Council	BB/I022570/1
European Research Council	700.58.305
???publication-publication-funding-organisation-not-added???	700.58.305

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

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10.1021/acs.jpclett.8b00108

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title = "Vibronic Coherence in the Charge Separation Process of the Rhodobacter sphaeroides Reaction Center",

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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AU - van Grondelle, Rienk

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

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