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Two-dimensional spectroscopy of electronic couplings in photosynthesis
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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“Microtubules in dendrites and nerve cell bodies are prevented from disassembly by microtubule associated proteins, rendering them more stable and able to encode the long-term information necessary to the theory of Orch OR 9,41,42 .”
From Quantum effects in the brain: A review (2020) · cites this paper as [9]
In the citing paper
“The predictions of Orch OR favour type A whereas actual mouse brain tissue points to the predominance of type B.”
From Quantum effects in the brain: A review (2020) · cites this paper as [9]
In the citing paper
“As outlined above, microtubule arrangement in the dendrites and cell bodies of nerve cells is suitable for information processing, making them a good contender for the biological site of consciousness 9,40,42 .”
From Quantum effects in the brain: A review (2020) · cites this paper as [9]
In the citing paper
“This is supported by the fact that certain chemicals that influence both consciousness as well as cognitive function, such as general anaesthetics and antidepressants, involve microtubules 9,61,62 .”
From Quantum effects in the brain: A review (2020) · cites this paper as [9]
In the citing paper
“The two-dimensional spectra revealed the presence of cross peaks [41] that oscillated in time [42].”
From The future of quantum biology (2018) · cites this paper as [41]
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Read, E. L., Engel, G. S., Calhoun, T. R., Mančal, T., Ahn, T. K., Blankenship, R. E., & Fleming, G. R. (2007) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0701201104 · Cited by 150
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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.
- Venue
- Nature
- Published
- 2005-03
- Volume
- 434
- Issue
- 7033
- Pages
- 625-628
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- 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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