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.
(Less)
- author
- Paleček, David
LU
; Edlund, Petra
; Westenhoff, Sebastian
LU
and Zigmantas, Donatas
LU
- organization
- publishing date
- 2017
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Science Advances
- volume
- 3
- issue
- 9
- article number
- 1603141
- publisher
- American Association for the Advancement of Science (AAAS)
- external identifiers
-
- scopus:85041698954
- pmid:28913419
- 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
- 2024-06-10 08:29:18
@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>}},
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}},
doi = {{10.1126/sciadv.1603141}},
volume = {{3}},
year = {{2017}},
}