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Cited by 56Spectroscopy and Quantum Chemical StudiesPhotochemistry and Electron Transfer StudiesPhotosynthetic Processes and Mechanisms

Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

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Perlík, Václav, Seibt, Joachim, Cranston, Laura J., Cogdell, Richard J., Lincoln, Craig N., Savolainen, Janne, Šanda, František, Mančal, Tomáš +1 more·2015·The Journal of Chemical Physics
DOI 10.1063/1.4919548
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Abstract

The initial energy transfer steps in photosynthesis occur on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which lead to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited states as part of the system’s Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid electronic ground state play the central role in the excited state population transfer to bacteriochlorophyll; resonance between the donor-acceptor energy gap and the vibrational ground state energies is the physical basis of the ultrafast energy transfer rates in these systems.

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  • A number of theoretical groups working on organic photovoltaics now apply an open-quantum systems approach, using methods strongly influenced by early studies of photosynthetic light-harvesting complexes.

    “A number of theoretical groups working on organic photovoltaics now apply an open-quantum systems approach, using methods strongly influenced by early studies of photosynthetic light-harvesting complexes [83 -86].”

    From The future of quantum biology (2018) · cites this paper as [83]

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Authors
Perlík, V., Seibt, J., Cranston, L. J., Cogdell, R. J., Lincoln, C. N., Savolainen, J., Šanda, F., Mančal, T., & Hauer, J.
Affiliations
  • Charles University (CZ)
  • University of Glasgow (GB)
  • TU Wien (AT)
  • Ruhr University Bochum (DE)
ORCID
Venue
The Journal of Chemical Physics
Publisher
AIP Publishing
Published
2015-05-04
Volume
142
Issue
21
Pages
212434-212434
ISSN
  • 0021-9606 (ISSN-L)
  • 1089-7690
DOI
10.1063/1.4919548
OpenAlex
W2108193123
Cited by
56
References
75
Citations by year
2025: 1 · 2024: 5 · 2023: 2 · 2022: 8 · 2021: 4 · 2020: 2 · 2019: 4 · 2018: 8 · 2017: 10 · 2016: 7 · 2015: 4 · 2013: 1
FWCI
4.91
Type
journal article
Language
en
Open access
Locations
  • The Journal of Chemical Physics (publishedVersion)
  • PubMed (publishedVersion)
  • arXiv (Cornell University) (submittedVersion)
  • arXiv (Cornell University)
Funders
  • Biotechnology and Biological Sciences Research Council
  • Austrian Science Fund (Y631-N27)
  • Czech Science Foundation (14-25752S)
Topics
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
  • Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
  • Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
Keywords
vibronic coupling, ultrafast energy transfer, photosynthetic light harvesting, LH2, Förster resonance, two-dimensional electronic spectroscopy, transient grating spectroscopy
MeSH terms
Bacteriochlorophylls, Carotenoids, Chromatium, Energy Transfer, Spectrum Analysis, Light-Harvesting Protein Complexes

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