Atomistic Study of the Long-Lived Quantum Coherences in the Fenna-Matthews-Olson Complex
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A remarkable amount of theoretical research has been carried out to elucidate the physical origins of the recently observed long-lived quantum coherence in the electronic energy transfer process in biological photosynthetic systems. Although successful in many respects, several widely used descriptions only include an effective treatment of the protein-chromophore interactions. In this work, by combining an all-atom molecular dynamics simulation, time-dependent density functional theory, and open quantum system approaches, we successfully simulate the dynamics of the electronic energy transfer of the Fenna-Matthews-Olson pigment-protein complex. The resulting characteristic beating of populations and quantum coherences is in good agreement with the experimental results and the hierarchy equation of motion approach. The experimental absorption, linear, and circular dichroism spectra and dephasing rates are recovered at two different temperatures. In addition, we provide an extension of our method to include zero-point fluctuations of the vibrational environment. This work thus presents, to our knowledge, one of the first steps to explain the role of excitonic quantum coherence in photosynthetic light-harvesting complexes based on their atomistic and molecular description.
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Under natural conditions a pigment-protein complex is not excited in an antisymmetric state but tends to receive a single excitation locally, for example on site 1 in the FMO complex.
“One may argue however, that under natural conditions a pigment-protein complex is not excited in such an antisymmetric state, but will tend to receive a single excitation locally, for example on site 1 (this is for example the case of the FMO complex [46]).”
From Vibrations, quanta and biology (2013) · cites this paper as [46]
Traditional perturbative treatments (Lindblad, Redfield, modified Redfield) do not well model structured environments and non-perturbative coupling.
“Both features are not well modeled by the traditional perturbative treatments that lead to master equations of Lindblad [139, 140], Redfield [141] or modified Redfield type [46, 142, 143] (see [60] for a review of master equations).”
From Vibrations, quanta and biology (2013) · cites this paper as [46]
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Self-citation
- Authors
- Shim, S., Rebentrost, P., Valleau, S., & Aspuru-Guzik, A.
- Affiliations
- Harvard University (US)
- Venue
- Biophysical Journal
- Publisher
- Elsevier BV
- Published
- 2012-02
- Volume
- 102
- Issue
- 3
- Pages
- 649-660
- ISSN
- 0006-3495 (ISSN-L)
- PMC
- PMC3274801
- OpenAlex
- W2082479893
- Cited by
- 219
- References
- 70
- Citations by year
- 2026: 4 · 2025: 3 · 2024: 12 · 2023: 2 · 2022: 8 · 2021: 7 · 2020: 7 · 2019: 15 · 2018: 11 · 2017: 19 · 2016: 20 · 2015: 17 · 2014: 27 · 2013: 28 · 2012: 38
- FWCI
- 18.21
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Licence
- Locations
- Biophysical Journal (publishedVersion)
- Europe PMC (PubMed Central) (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- Digital Access to Scholarship at Harvard (DASH) (Harvard University) (submittedVersion, cc-by)
- arXiv (Cornell University)
- Funders
- U.S. Department of Energy (DESC0001088)
- 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 › Strong Light-Matter Interactions
- Keywords
- Fenna-Matthews-Olson complex, excitation energy transfer, light-harvesting complexes, chromophore-protein interaction, open quantum systems, dephasing rate, circular dichroism, linear dichroism, molecular dynamics
- MeSH terms
- Bacterial Proteins, Electrons, Energy Transfer, Pigments, Biological, Quantum Theory, Temperature, Time Factors, Light-Harvesting Protein Complexes, Molecular Dynamics Simulation
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