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  Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

Duan, H.-G., Prokhorenko, V., Cogdell, R., Ashraf, K., Stevens, A., Thorwart, M., et al. (2017). Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer. Proceedings of the National Academy of Sciences of the United States of America, 114(32), 8493-8498. doi:10.1073/pnas.1702261114.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002B-B9B3-6 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-EA61-A
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http://arxiv.org/abs/1610.08425 (Preprint)
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Supporting Information Appendix.

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 Creators:
Duan, Hong-Guang1, 2, 3, Author              
Prokhorenko, Valentyn1, Author              
Cogdell, Richard4, Author
Ashraf, Khuram4, Author
Stevens, Amy1, 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              
4Institute of Molecular, Cell and Systems Biology, College of Medical, Veterinary and Life Science, University of Glasgow, Glasgow G12 8QQ, UK, ou_persistent22              
5The Departments of Chemistry and Physics, University of Toronto, 80 St. George Street, Toronto Canada M5S 3H6, ou_persistent22              

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Free keywords: Biological Physics; Chemical Physics; Quantum Physics
 Abstract: During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is understood in terms of exciton quasiparticles which move on a grid of biomolecular sites on typical time scales less than 100 femtoseconds (fs). Since the early days of quantum mechanics, this energy transfer is described as an incoherent Forster hopping with classical site occupation probabilities, but with quantum mechanically determined rate constants. This orthodox picture has been challenged by ultrafast optical spectroscopy experiments with the Fenna-Matthews-Olson protein in which interference oscillatory signals up to 1.5 picoseconds were reported and interpreted as direct evidence of exceptionally long-lived electronic quantum coherence. Here, we show that the optical 2D photon echo spectra of this complex at ambient temperature in aqueous solution do not provide evidence of any long-lived electronic quantum coherence, but confirm the orthodox view of rapidly decaying electronic quantum coherence on a time scale of 60 fs. Our results give no hint that electronic quantum coherence plays any biofunctional role in real photoactive biomolecular complexes. Since this natural energy transfer complex is rather small and has a structurally well defined protein with the distances between bacteriochlorophylls being comparable to other light-harvesting complexes, we anticipate that this finding is general and directly applies to even larger photoactive biomolecular complexes.

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Language(s): eng - English
 Dates: 2016-10-262017-02-092017-06-012017-07-252017-08-08
 Publication Status: Published in print
 Pages: 6
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: arXiv: 1610.08425
DOI: 10.1073/pnas.1702261114
 Degree: -

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Title: Proceedings of the National Academy of Sciences of the United States of America
  Other : Proceedings of the National Academy of Sciences of the USA
  Other : Proc. Acad. Sci. USA
  Other : Proc. Acad. Sci. U.S.A.
  Abbreviation : PNAS
Source Genre: Journal
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Publ. Info: Washington, D.C. : National Academy of Sciences
Pages: 6 Volume / Issue: 114 (32) Sequence Number: - Start / End Page: 8493 - 8498 Identifier: ISSN: 0027-8424
CoNE: /journals/resource/954925427230