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Cited by 1,241Spectroscopy and Quantum Chemical StudiesPhotochemistry and Electron Transfer StudiesLaser-Matter Interactions and Applications

The DOI matches its Crossref record; 31 of the 31 references it cites were found in a registry or an index.

Two-dimensional spectroscopy of electronic couplings in photosynthesis

Brixner, Tobias, Stenger, Jens, Vaswani, Harsha M., Cho, Minhaeng, Blankenship, Robert E., Fleming, Graham R.·2005·Nature
DOI 10.1038/nature03429
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Abstract

Time-resolved optical spectroscopy is widely used to study vibrational and electronic dynamics by monitoring transient changes in excited state populations on a femtosecond timescale. Yet the fundamental cause of electronic and vibrational dynamics--the coupling between the different energy levels involved--is usually inferred only indirectly. Two-dimensional femtosecond infrared spectroscopy based on the heterodyne detection of three-pulse photon echoes has recently allowed the direct mapping of vibrational couplings, yielding transient structural information. Here we extend the approach to the visible range and directly measure electronic couplings in a molecular complex, the Fenna-Matthews-Olson photosynthetic light-harvesting protein. As in all photosynthetic systems, the conversion of light into chemical energy is driven by electronic couplings that ensure the efficient transport of energy from light-capturing antenna pigments to the reaction centre. We monitor this process as a function of time and frequency and show that excitation energy does not simply cascade stepwise down the energy ladder. We find instead distinct energy transport pathways that depend sensitively on the detailed spatial properties of the delocalized excited-state wavefunctions of the whole pigment-protein complex.

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Crossref · 10.1038/nature03429

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  1. Zewail, A. H. Femtochemistry (World Scientific, Singapore, 1994)

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Metadata

Authors
Brixner, T., Stenger, J., Vaswani, H. M., Cho, M., Blankenship, R. E., & Fleming, G. R.
Affiliations
  • QB3 (US)
  • Korea University (KR)
  • Arizona State University (US)
Corresponding author
  • Cho, Minhaeng
  • Fleming, Graham R.
ORCID
Venue
Nature
Publisher
Springer Science and Business Media LLC
Published
2005-03
Volume
434
Issue
7033
Pages
625-628
ISSN
  • 0028-0836 (ISSN-L)
  • 1476-4687
DOI
10.1038/nature03429
OpenAlex
W2088307177
Cited by
1,241
References
31
Citations by year
2026: 30 · 2025: 40 · 2024: 33 · 2023: 40 · 2022: 37 · 2021: 51 · 2020: 51 · 2019: 58 · 2018: 66 · 2017: 66 · 2016: 65 · 2015: 75 · 2014: 68 · 2013: 102 · 2012: 60
FWCI
37.16
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)
Funders
  • U.S. Department of Energy
  • University of California Berkeley
  • Arizona State University
  • Korea Science and Engineering Foundation
  • Office of Science
  • Los Alamos National Laboratory
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
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
Keywords
electronic coupling, Fenna-Matthews-Olson complex, photosynthetic light harvesting, two-dimensional spectroscopy, femtosecond infrared spectroscopy, photon echo, pigment-protein complexes, excitation energy transfer
MeSH terms
Bacterial Proteins, Electron Transport, Light, Models, Chemical, Models, Molecular, Photosynthesis, Protein Conformation, Protons, Spectrum Analysis, Time Factors, Vibration, Chlorobium, Light-Harvesting Protein Complexes

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