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Quantum coherence as a witness of vibronically hot energy transfer in bacterial reaction center

Paleček, David LU ; Edlund, Petra; Westenhoff, Sebastian LU and Zigmantas, Donatas LU (2017) In Science Advances 3(9).
Abstract

Photosynthetic proteins have evolved over billions of years so as to undergo optimal energy transfer to the sites of charge separation. On the basis of spectroscopically detected quantum coherences, it has been suggested that this energy transfer is partially wavelike. This conclusion depends critically on the assignment of the coherences to the evolution of excitonic superpositions. We demonstrate that, for a bacterial reaction center protein, long-lived coherent spectroscopic oscillations, which bear canonical signatures of excitonic superpositions, are essentially vibrational excited-state coherences shifted to the ground state of the chromophores. We show that the appearance of these coherences arises from a release of electronic... (More)

Photosynthetic proteins have evolved over billions of years so as to undergo optimal energy transfer to the sites of charge separation. On the basis of spectroscopically detected quantum coherences, it has been suggested that this energy transfer is partially wavelike. This conclusion depends critically on the assignment of the coherences to the evolution of excitonic superpositions. We demonstrate that, for a bacterial reaction center protein, long-lived coherent spectroscopic oscillations, which bear canonical signatures of excitonic superpositions, are essentially vibrational excited-state coherences shifted to the ground state of the chromophores. We show that the appearance of these coherences arises from a release of electronic energy during energy transfer. Our results establish how energy migrates on vibrationally hot chromophores in the reaction center, and they call for a reexamination of claims of quantum energy transfer in photosynthesis.

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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Science Advances
volume
3
issue
9
publisher
American Association for the Advancement of Science (AAAS)
external identifiers
  • scopus:85041698954
ISSN
2375-2548
DOI
10.1126/sciadv.1603141
language
English
LU publication?
yes
id
c05bee5b-1ce5-46a6-920f-ab17b193ee44
date added to LUP
2018-02-23 15:36:21
date last changed
2018-07-08 04:30:13
@article{c05bee5b-1ce5-46a6-920f-ab17b193ee44,
  abstract     = {<p>Photosynthetic proteins have evolved over billions of years so as to undergo optimal energy transfer to the sites of charge separation. On the basis of spectroscopically detected quantum coherences, it has been suggested that this energy transfer is partially wavelike. This conclusion depends critically on the assignment of the coherences to the evolution of excitonic superpositions. We demonstrate that, for a bacterial reaction center protein, long-lived coherent spectroscopic oscillations, which bear canonical signatures of excitonic superpositions, are essentially vibrational excited-state coherences shifted to the ground state of the chromophores. We show that the appearance of these coherences arises from a release of electronic energy during energy transfer. Our results establish how energy migrates on vibrationally hot chromophores in the reaction center, and they call for a reexamination of claims of quantum energy transfer in photosynthesis.</p>},
  articleno    = {1603141},
  author       = {Paleček, David and Edlund, Petra and Westenhoff, Sebastian and Zigmantas, Donatas},
  issn         = {2375-2548},
  language     = {eng},
  number       = {9},
  publisher    = {American Association for the Advancement of Science (AAAS)},
  series       = {Science Advances},
  title        = {Quantum coherence as a witness of vibronically hot energy transfer in bacterial reaction center},
  url          = {http://dx.doi.org/10.1126/sciadv.1603141},
  volume       = {3},
  year         = {2017},
}