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The fundamental role of quantized vibrations in coherent light harvesting by cryptophyte algae
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The influence of fast vibrations on energy transfer and conversion in natural molecular aggregates is an issue of central interest. This article shows the important role of high-energy quantized vibrations and their non-equilibrium dynamics for energy transfer in photosynthetic systems with highly localized excitonic states. We consider the cryptophyte antennae protein phycoerythrin 545 and show that coupling to quantized vibrations, which are quasi-resonant with excitonic transitions is fundamental for biological function as it generates non-cascaded transport with rapid and wider spatial distribution of excitation energy. Our work also indicates that the non-equilibrium dynamics of such vibrations can manifest itself in ultrafast beating of both excitonic populations and coherences at room temperature, with time scales in agreement with those reported in experiments. Moreover, we show that mechanisms supporting coherent excitonic dynamics assist coupling to selected modes that channel energy to preferential sites in the complex. We therefore argue that, in the presence of strong coupling between electronic excitations and quantized vibrations, a concrete and important advantage of quantum coherent dynamics is precisely to tune resonances that promote fast and effective energy distribution.
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“The environmental spectral densities [25] describing their interaction with the system tend to display two principal structures, a broad smooth background which has a short memory time and interacts with the system mainly through its fluctuations, i.e. causing noise, and well defined narrow features corresponding, for example, to long-lived vibrational motion that can lead to quasi-coherent Dynami”
From Vibrations, quanta and biology (2013) · cites this paper as [25]
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Maiuri, M., Oviedo, M. B., Dean, J. C., Bishop, M. M., Kudisch, B. J., Toa, Z. S. D., Wong, B. M., McGill, S., & Scholes, G. D. (2018) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.8b02748 · Cited by 25
Self-citationPrior, J., Castro, E., Chin, A. W., Almeida, J., Huelga, S. F., & Plenio, M. B. (2013) · The Journal of Chemical Physics · doi:10.1063/1.4837718 · Cited by 24
Simulating Quantum Vibronic Dynamics at Finite Temperatures With Many Body Wave Functions at 0 K
Dunnett, A., & Chin, A. W. (2021) · Frontiers in Chemistry · doi:10.3389/fchem.2020.600731 · Cited by 27
“In many molecular systems—and particularly biological systems where the transfer between electronic states is affected by coupling to chromophore and protein modes—the systembath physics is highly non-perturbative and J(ω) has very sharp frequency-dependence (May and Kühn, 2008; Womick et al., 2011; Kolli et al., 2012…”
BackgroundLai, Y., & Geva, E. (2021) · The Journal of Chemical Physics · doi:10.1063/5.0069313 · Cited by 23
Lewis, N. H. C., Dong, H., Oliver, T. A. A., & Fleming, G. R. (2015) · The Journal of Chemical Physics · doi:10.1063/1.4931634 · Cited by 25
Pseudomode Approach and Vibronic Non-Markovian Phenomena in Light-Harvesting Complexes
Teretenkov, A. E. (2019) · Proceedings of the Steklov Institute of Mathematics · doi:10.1134/s0081543819050201 · Cited by 22
Estimation of damped oscillation associated spectra from ultrafast transient absorption spectra
van Stokkum, I. H. M., Jumper, C. C., Snellenburg, J. J., Scholes, G. D., van Grondelle, R., & Malý, P. (2016) · The Journal of Chemical Physics · doi:10.1063/1.4966196 · Cited by 24
Self-citation
Metadata
- Authors
- Kolli, A., O’Reilly, E. J., Scholes, G. D., & Olaya-Castro, A.
- Affiliations
- University College London (GB)
- University of Toronto (CA)
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2012-11-06
- Volume
- 137
- Issue
- 17
- Pages
- 174109-174109
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W1991695217
- Cited by
- 219
- References
- 49
- Citations by year
- 2026: 4 · 2025: 4 · 2024: 9 · 2023: 7 · 2022: 13 · 2021: 13 · 2020: 10 · 2019: 17 · 2018: 16 · 2017: 23 · 2016: 28 · 2015: 34 · 2014: 18 · 2013: 20 · 2012: 2
- FWCI
- 12.23
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- The Journal of Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- UCL Discovery (University College London) (submittedVersion)
- arXiv (Cornell University)
- Funders
- Engineering and Physical Sciences Research Council (EP/G005222/1)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Strong Light-Matter Interactions
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Keywords
- cryptophyte algae, excitonic energy transfer, excitonic coherence, ultrafast exciton dynamics, exciton-vibration coupling, photosynthetic antenna proteins, resonant frequency tuning
- MeSH terms
- Electrons, Energy Transfer, Models, Molecular, Phycoerythrin, Protein Conformation, Quantum Theory, Vibration, Cryptophyta
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