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  Quantum coherent energy transport in the Fenna–Matthews–Olson complex at low temperature

Duan, H.-G., Jha, A., Chen, L., Tiwari, V., Cogdell, R. J., Ashraf, K., et al. (2022). Quantum coherent energy transport in the Fenna–Matthews–Olson complex at low temperature. Proceedings of the National Academy of Sciences of the United States of America, 119(49): e2212630119. doi:10.1073/pnas.2212630119.

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 Creators:
Duan, H.-G.1, 2, 3, 4, Author           
Jha, A.2, 5, 6, Author           
Chen, L.7, 8, Author
Tiwari, V.2, 9, 10, Author           
Cogdell, R. J.11, Author
Ashraf, K.11, Author
Prokhorenko, V.2, Author           
Thorwart, M.3, 4, Author
Miller, R. J. D.12, 13, Author
Affiliations:
1Department of Physics, School of Physical Science and Technology, Ningbo University, ou_persistent22              
2Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
3I. Institut für Theoretische Physik, Universität Hamburg , ou_persistent22              
4The Hamburg Center for Ultrafast Imaging, ou_persistent22              
5The Rosalind Franklin Institute, Rutherford Appleton Laboratory, Harwell Campus, ou_persistent22              
6Research Complex at Harwell, Rutherford Appleton Laboratory, ou_persistent22              
7Zhejiang Laboratory, ou_persistent22              
8Department of Chemistry, Technische Universität München, ou_persistent22              
9Department of Chemistry, Universität Hamburg, ou_persistent22              
10European XFEL GmbH , ou_persistent22              
11School of Molecular Biosciences, University of Glasgow , ou_persistent22              
12Department of Chemistry, University of Toronto, ou_persistent22              
13Department of Physics, University of Toronto, ou_persistent22              

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Free keywords: energy transfer; two-dimensional spectroscopy; excitonic coupling; coherent transp
 Abstract: In the primary step of natural light harvesting, the solar photon energy is captured in a photoexcited electron–hole pair, or an exciton, in chlorophyll. Its conversion to chemical potential occurs in the special pair reaction center, which is reached by downhill ultrafast excited-state energy transport through a network of chromophores. Being inherently quantum, transport could in principle occur via a matter wave, with vast implications for efficiency. How long a matter wave remains coherent is determined by the intensity by which the exciton is disturbed by the noisy biological environment. The stronger this is, the stronger the electronic coupling between chromophores must be to overcome the fluctuations and phase shifts. The current consensus is that under physiological conditions, quantum coherence vanishes on the 10-fs time scale, rendering it irrelevant for the observed picosecond transfer. Yet, at low-enough temperature, quantum coherence should in principle be present. Here, we reveal the onset of longer-lived electronic coherence at extremely low temperatures of ∼20 K. Using two-dimensional electronic spectroscopy, we determine the exciton coherence times in the Fenna–Matthew–Olson complex over an extensive temperature range. At 20 K, coherence persists out to 200 fs (close to the antenna) and marginally up to 500 fs at the reaction center. It decays markedly faster with modest increases in temperature to become irrelevant above 150 K. At low temperature, the fragile electronic coherence can be separated from the robust vibrational coherence, using a rigorous theoretical analysis. We believe that by this generic principle, light harvesting becomes robust against otherwise fragile quantum effects.

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Language(s): eng - English
 Dates: 2022-07-222022-10-182022-11-282022-12-06
 Publication Status: Issued
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1073/pnas.2212630119
arXiv: 2104.01462
 Degree: -

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Project name : This work was supported by the Max Planck Society and the Excellence Cluster “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG)–EXC 2056–project ID 390715994. K.A. and R.J.C. acknowledge funding by “The Photosynthetic Antenna Research Center” under the US DoE Energy Frontier Research Center grant number DE-SC 0001035. Lipeng Chen was supported by the Key Research Project of Zhejiang Lab (No. 2021PE0AC02).
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Title: Proceedings of the National Academy of Sciences of the United States of America
  Other : PNAS
  Other : Proceedings of the National Academy of Sciences of the USA
  Abbreviation : Proc. Natl. Acad. Sci. U. S. A.
Source Genre: Journal
 Creator(s):
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Publ. Info: Washington, D.C. : National Academy of Sciences
Pages: - Volume / Issue: 119 (49) Sequence Number: e2212630119 Start / End Page: - Identifier: ISSN: 0027-8424
CoNE: https://pure.mpg.de/cone/journals/resource/954925427230