ArticleProceedings of the National Academy of Sciences of the United States of America2018
Local protein solvation drives direct down-conversion in phycobiliprotein PC645 via incoherent vibronic transport.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2018. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 22 papers.
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22 citing papers in PubMed, 92 citations in OpenAlex.
- pH-Dependent Vibrational Dynamics Drives Excited-State Quenching in the Phycobiliprotein Complex PC645.Journal of the American Chemical Society · 2026Article
- Minimization of Disorder as a Key Design Principle for Natural Sizes of Light Harvesting 2 Complexes.The journal of physical chemistry letters · 2026Article
- Convenient Preparation and Energy Transfer Kinetic Process Verification by Ultrafast Time-resolved Fluorescence Spectra for Natural Cryptophyte Phycocyanin 645.Journal of fluorescence · 2026Article
- Trajectory-based computational analysis of the quantum-classical transition in asymmetrically coupled spin-boson models.Computational and structural biotechnology journal · 2026Article
- Dissipation Pathways in a Photosynthetic Complex.The journal of physical chemistry letters · 2025Article
- Full microscopic simulations uncover persistent quantum effects in primary photosynthesis.Science advances · 2025Article
- Improved Description of Environment and Vibronic Effects with Electrostatically Embedded ML Potentials.The journal of physical chemistry letters · 2025Article
- Ultrafast exciton energy transfer dynamics in the cryptophyte light-harvesting antenna phycoerythrin 566.Frontiers in plant science · 2025Article
- Reversible disassembly-reassembly of C-phycocyanin in pressurization-depressurization cycles of high hydrostatic pressure.International journal of biological macromolecules · 2023Article
- Mapping electronic decoherence pathways in molecules.Proceedings of the National Academy of Sciences of the United States of America · 2023Article
- Resonant vibrations produce quantum bridge over high-energy states in heterogeneous antenna.Photosynthesis research · 2023Article
- Infrared Signatures of Phycobilins within the Phycocyanin 645 Complex.The journal of physical chemistry. B · 2023Article
- Recent progress in atomistic modeling of light-harvesting complexes: a mini review.Photosynthesis research · 2023Review
- Unraveling the role of thermal fluctuations on the exciton structure of the cryptophyte PC612 and PC645 photosynthetic antenna complexes.Frontiers in molecular biosciences · 2023Article
- Exact simulation of pigment-protein complexes unveils vibronic renormalization of electronic parameters in ultrafast spectroscopy.Nature communications · 2022Article
- Formally exact simulations of mesoscale exciton dynamics in molecular materials.Chemical science · 2021Article
- Semiclassical Modified Redfield and Generalized Förster Theories of Exciton Relaxation/Transfer in Light-Harvesting Complexes: The Quest for the Principle of Detailed Balance.The journal of physical chemistry. B · 2021Article
- Machine-learned potentials for next-generation matter simulations.Nature materials · 2021Review
- Photosynthesis tunes quantum-mechanical mixing of electronic and vibrational states to steer exciton energy transfer.Proceedings of the National Academy of Sciences of the United States of America · 2021Article
- Static Disorder in Excitation Energies of the Fenna-Matthews-Olson Protein: Structure-Based Theory Meets Experiment.The journal of physical chemistry letters · 2020Article
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Authors and funding
5 authors at 3 institutions in 2 countries.
Funding
No grant is acknowledged in the PubMed record.
Abstract
The mechanisms controlling excitation energy transport (EET) in light-harvesting complexes remain controversial. Following the observation of long-lived beats in 2D electronic spectroscopy of PC645, vibronic coherence, the delocalization of excited states between pigments supported by a resonant vibration, has been proposed to enable direct excitation transport from the highest-energy to the lowest-energy pigments, bypassing a collection of intermediate states. Here, we instead show that for phycobiliprotein PC645 an incoherent vibronic transport mechanism is at play. We quantify the solvation dynamics of individual pigments using ab initio quantum mechanics/molecular mechanics (QM/MM) nuclear dynamics. Our atomistic spectral densities reproduce experimental observations ranging from absorption and fluorescence spectra to the timescales and selectivity of down-conversion observed in transient absorption measurements. We construct a general model for vibronic dimers and establish the parameter regimes of coherent and incoherent vibronic transport. We demonstrate that direct down-conversion in PC645 proceeds incoherently, enhanced by large reorganization energies and a broad collection of high-frequency vibrations. We suggest that a similar incoherent mechanism is appropriate across phycobiliproteins and represents a potential design principle for nanoscale control of EET.
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