Electronic resonance with anticorrelated pigment vibrations drives photosynthetic energy transfer outside the adiabatic framework
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The delocalized, anticorrelated component of pigment vibrations can drive nonadiabatic electronic energy transfer in photosynthetic light-harvesting antennas. In femtosecond experiments, this energy transfer mechanism leads to excitation of delocalized, anticorrelated vibrational wavepackets on the ground electronic state that exhibit not only 2D spectroscopic signatures attributed to electronic coherence and oscillatory quantum energy transport but also a cross-peak asymmetry not previously explained by theory. A number of antennas have electronic energy gaps matching a pigment vibrational frequency with a small vibrational coordinate change on electronic excitation. Such photosynthetic energy transfer steps resemble molecular internal conversion through a nested intermolecular funnel.
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The sharp features tend to originate from long-lived vibrations that belong to molecules held within the protein scaffold.
“As we will see later the smooth background is due mostly to the protein environment as well as noise processes originating from solvents while the sharp features tend to originate from long-lived vibrations that belong to molecules that are held within the protein scaffold [26, 27].”
From Vibrations, quanta and biology (2013) · cites this paper as [26]
The smooth background is due mostly to the protein environment and noise processes from solvents.
“As we will see later the smooth background is due mostly to the protein environment as well as noise processes originating from solvents while the sharp features tend to originate from long-lived vibrations that belong to molecules that are held within the protein scaffold [26, 27].”
From Vibrations, quanta and biology (2013) · cites this paper as [26]
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- Authors
- Tiwari, V., Peters, W. K., & Jonas, D. M.
- Affiliations
- University of Colorado Boulder (US)
- Venue
- Proceedings of the National Academy of Sciences
- Publisher
- National Academy of Sciences
- Published
- 2012-12-24
- Volume
- 110
- Issue
- 4
- Pages
- 1203-1208
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- PMC
- PMC3557059
- OpenAlex
- W2066289545
- Cited by
- 566
- References
- 36
- Citations by year
- 2026: 21 · 2025: 33 · 2024: 29 · 2023: 42 · 2022: 31 · 2021: 29 · 2020: 34 · 2019: 49 · 2018: 50 · 2017: 57 · 2016: 42 · 2015: 55 · 2014: 50 · 2013: 41
- FWCI
- 24.13
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- Proceedings of the National Academy of Sciences (publishedVersion)
- Europe PMC (PubMed Central) (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- Funders
- National Science Foundation (1112365, 0821794)
- National Center for Atmospheric Research (CNS-0821794)
- University of Colorado Boulder (CNS-0821794)
- University of Colorado Denver (CNS-0821794)
- Division of Chemistry (CHE-1112365)
- 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
- photosynthetic energy transfer, vibrational wave packets, 2D spectroscopy, electronic coherence, light-harvesting antenna, internal conversion
- MeSH terms
- Electron Transport, Electrons, Energy Transfer, Models, Biological, Photosynthesis, Quantum Theory, Spectrum Analysis, Vibration, Photosynthetic Reaction Center Complex Proteins
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