Cited by 3,315Spectroscopy and Quantum Chemical StudiesPhotosynthetic Processes and MechanismsPhotochemistry and Electron Transfer Studies

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Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems

Engel, Gregory S., Calhoun, Tessa R., Read, Elizabeth L., Ahn, Tae-Kyu, Mančal, Tomáš, Cheng, Yuan-Chung, Blankenship, Robert E., Fleming, Graham R.·2007·Nature

DOI 10.1038/nature05678

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Abstract

Photosynthetic complexes are exquisitely tuned to capture solar light efficiently, and then transmit the excitation energy to reaction centres, where long term energy storage is initiated. The energy transfer mechanism is often described by semiclassical models that invoke 'hopping' of excited-state populations along discrete energy levels. Two-dimensional Fourier transform electronic spectroscopy has mapped these energy levels and their coupling in the Fenna-Matthews-Olson (FMO) bacteriochlorophyll complex, which is found in green sulphur bacteria and acts as an energy 'wire' connecting a large peripheral light-harvesting antenna, the chlorosome, to the reaction centre. The spectroscopic data clearly document the dependence of the dominant energy transport pathways on the spatial properties of the excited-state wavefunctions of the whole bacteriochlorophyll complex. But the intricate dynamics of quantum coherence, which has no classical analogue, was largely neglected in the analyses-even though electronic energy transfer involving oscillatory populations of donors and acceptors was first discussed more than 70 years ago, and electronic quantum beats arising from quantum coherence in photosynthetic complexes have been predicted and indirectly observed. Here we extend previous two-dimensional electronic spectroscopy investigations of the FMO bacteriochlorophyll complex, and obtain direct evidence for remarkably long-lived electronic quantum coherence playing an important part in energy transfer processes within this system. The quantum coherence manifests itself in characteristic, directly observable quantum beating signals among the excitons within the Chlorobium tepidum FMO complex at 77 K. This wavelike characteristic of the energy transfer within the photosynthetic complex can explain its extreme efficiency, in that it allows the complexes to sample vast areas of phase space to find the most efficient path.

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Authors: Engel, G. S., Calhoun, T. R., Read, E. L., Ahn, T.-K., Mančal, T., Cheng, Y.-C., Blankenship, R. E., & Fleming, G. R.
Affiliations: QB3 (US)
Washington University in St. Louis (US)
Corresponding author: Fleming, Graham R.
ORCID: Engel, Gregory S.
Calhoun, Tessa R.
Read, Elizabeth L.
Mančal, Tomáš
Cheng, Yuan-Chung
Blankenship, Robert E.
Fleming, Graham R.
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2007-04
Volume: 446
Issue: 7137
Pages: 782-786
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/nature05678
OpenAlex: W2058468006
Cited by: 3,315
References: 31
Citations by year: 2026: 158 · 2025: 164 · 2024: 142 · 2023: 118 · 2022: 137 · 2021: 144 · 2020: 168 · 2019: 177 · 2018: 173 · 2017: 214 · 2016: 225 · 2015: 202 · 2014: 229 · 2013: 247 · 2012: 210
FWCI: 73.11
Type: journal article
Language: en
Open access: closed
Licence: www.springer.com/tdm (tdm)
Locations: Nature (publishedVersion)
PubMed (publishedVersion)
RePEc: Research Papers in Economics (submittedVersion)
Topics: Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
Keywords: quantum beats, exciton transfer, light-harvesting complexes, two-dimensional electronic spectroscopy, Chlorobium tepidum, green sulfur bacteria, Fenna-Matthews-Olson complex, long-lived coherence, energy transfer efficiency, exciton dynamics, phase space sampling
MeSH terms: Bacterial Proteins, Electron Transport, Electrons, Photosynthesis, Spectrum Analysis, Chlorobi, Chlorobium, Light-Harvesting Protein Complexes

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Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems

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