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

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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: Brixner, Tobias
Cho, Minhaeng
Blankenship, Robert E.
Fleming, Graham R.
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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Two-dimensional spectroscopy of electronic couplings in photosynthesis

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