Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 17, Issue 46, Pages 30828-30841Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5cp00582e
Keywords
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Funding
- Dutch Foundation for Basic Research (NWO) [040.11.428]
- Russian Foundation for Basic Research [15-04-02136]
- VU University Amsterdam
- Laserlab-Europe Consortium
- TOP grant from the Foundation of Chemical Sciences part of NWO [700.58.305]
- European Research Council [267333]
- EU FP7 project PAPETS [GA 323901]
- Netherlands Royal Academy of Sciences (KNAW)
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In photosynthesis absorbed sun light produces collective excitations (excitons) that form a coherent superposition of electronic and vibrational states of the individual pigments. Two-dimensional (2D) electronic spectroscopy allows a visualization of how these coherences are involved in the primary processes of energy and charge transfer. Based on quantitative modeling we identify the exciton-vibrational coherences observed in 2D photon echo of the photosystem II reaction center (PSII-RC). We find that the vibrations resonant with the exciton splittings can modify the delocalization of the exciton states and produce additional states, thus promoting directed energy transfer and allowing a switch between the two charge separation pathways. We conclude that the coincidence of the frequencies of the most intense vibrations with the splittings within the manifold of exciton and charge-transfer states in the PSII-RC is not occurring by chance, but reflects a fundamental principle of how energy conversion in photosynthesis was optimized.
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