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

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Duan,  Hong-Guang
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
I. Institut für Theoretische Physik, Universität Hamburg;
The Hamburg Center for Ultrafast Imaging;

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Prokhorenko,  Valentyn
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

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Miller,  R. J. Dwayne
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
The Hamburg Center for Ultrafast Imaging;
The Departments of Chemistry and Physics, University of Toronto;

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Zitation

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. doi:10.1038/s41598-017-12564-4.


Zitierlink: https://hdl.handle.net/11858/00-001M-0000-002E-7F9F-1
Zusammenfassung
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.