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  Primary Charge Separation in the Photosystem II Reaction Center Revealed by a Global Analysis of the Two-dimensional Electronic Spectra

Duan, H.-G., Prokhorenko, V., Wientjes, E., Croce, R., Thorwart, M., & Miller, R. J. D. (2017). Primary Charge Separation in the Photosystem II Reaction Center Revealed by a Global Analysis of the Two-dimensional Electronic Spectra. Scientific Reports, 7: 12347. doi:10.1038/s41598-017-12564-4.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002E-7F9F-1 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-EAD0-C
Genre: Journal Article

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https://dx.doi.org/10.1038/s41598-017-12564-4 (Publisher version)
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 Creators:
Duan, Hong-Guang1, 2, 3, Author              
Prokhorenko, Valentyn1, Author              
Wientjes, Emilie 4, Author
Croce, Roberta4, Author
Thorwart, Michael2, 3, Author
Miller, R. J. Dwayne1, 3, 5, Author              
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2I. Institut für Theoretische Physik, Universität Hamburg, Jungiusstraße 9, 20355, Hamburg, Germany, ou_persistent22              
3The Hamburg Center for Ultrafast Imaging, Luruper Chaussee 149, 22761, Hamburg, Germany, ou_persistent22              
4Department of Physics and Astronomy and Institute for Lasers, Life and Biophotonics, Faculty of Sciences, VU University Amsterdam, De Boelelaan, 1081, 1081, HV, Amsterdam, The Netherlands, ou_persistent22              
5The Departments of Chemistry and Physics, University of Toronto, 80 St. George Street, Toronto, M5S 3H6, Canada, ou_persistent22              

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Free keywords: Chemical physics; Light harvesting
 Abstract: The transfer of electronic charge in the reaction center of Photosystem II is one of the key building blocks of the conversion of sunlight energy into chemical energy within the cascade of the photosynthetic reactions. Since the charge transfer dynamics is mixed with the energy transfer dynamics, an effective tool for the direct resolution of charge separation in the reaction center is still missing. Here, we use experimental two-dimensional optical photon echo spectroscopy in combination with the theoretical calculation to resolve its signature. A global fitting analysis allows us to clearly and directly identify a decay pathway associated to the primary charge separation. In particular, it can be distinguished from regular energy transfer and occurs on a time scale of 1.5 ps under ambient conditions. This technique provides a general tool to identify charge separation signatures from the energy transport in two-dimensional optical spectroscopy.

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Language(s): eng - English
 Dates: 2017-03-292017-09-122017-09-27
 Publication Status: Published online
 Pages: -
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 Rev. Method: Peer
 Identifiers: DOI: 10.1038/s41598-017-12564-4
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Title: Scientific Reports
  Abbreviation : Sci. Rep.
Source Genre: Journal
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Publ. Info: London, UK : Nature Publishing Group
Pages: - Volume / Issue: 7 Sequence Number: 12347 Start / End Page: - Identifier: ISSN: 2045-2322
CoNE: /journals/resource/2045-2322