ArticleThe journal of physical chemistry. B2021
Semiclassical Modified Redfield and Generalized Förster Theories of Exciton Relaxation/Transfer in Light-Harvesting Complexes: The Quest for the Principle of Detailed Balance.
Article in The journal of physical chemistry. B, 2021. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 10 papers.
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10 citing papers in PubMed.
- Article
- pH-Dependent Vibrational Dynamics Drives Excited-State Quenching in the Phycobiliprotein Complex PC645.Journal of the American Chemical Society · 2026Article
- Nuclear quantum effects slow down the energy transfer in biological light-harvesting complexes.Science advances · 2025Article
- Exciton dynamics from the mapping approach to surface hopping: comparison with Förster and Redfield theories.Physical chemistry chemical physics : PCCP · 2024Article
- Gaussian Decomposition vs. Semiclassical Quantum Simulation: Obtaining the High-Order Derivatives of a Spectrum in the Case of Photosynthetic Pigment Optical Properties Studying.Sensors (Basel, Switzerland) · 2023Article
- Unravelling the Roles of Integral Polypeptides in Excitation Energy Transfer of Photosynthetic RC-LH1 Supercomplexes.The journal of physical chemistry. B · 2023Article
- Living on the edge: light-harvesting efficiency and photoprotection in the core of green sulfur bacteria.Physical chemistry chemical physics : PCCP · 2023Article
- Tight inner ring architecture and quantum motion of nuclei enable efficient energy transfer in bacterial light harvesting.Science advances · 2022Article
- Explaining the Efficiency of Photosynthesis: Quantum Uncertainty or Classical Vibrations?The journal of physical chemistry letters · 2022Article
- The Relationship between the Spatial Arrangement of Pigments and Exciton Transition Moments in Photosynthetic Light-Harvesting Complexes.International journal of molecular sciences · 2021Article
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Abstract
A conceptual problem of transfer theories that use a semiclassical description of the electron-vibrational coupling is the neglect of the correlation between momenta and coordinates of nuclei. In the Redfield theory of exciton relaxation, this neglect leads to a violation of the principle of detailed balance; equal "uphill" and "downhill" transfer rate constants are obtained. Here, we investigate how this result depends on nuclear reorganization effects, neglected in Redfield but taken into account in the modified Redfield theory. These reorganization effects, resulting from a partial localization of excited states, are found to promote a preferential "downhill" relaxation of excitation energy. However, for realistic spectral densities of light-harvesting antennae in photosynthesis, the reorganization effects are too small to compensate for the missing coordinate-momentum uncertainty. For weaker excitonic couplings as they occur between domains of strongly coupled pigments, we find the principle of detailed balance to be fulfilled in a semiclassical variant of the generalized Förster theory. A qualitatively correct description of the transfer is obtained with this theory at a significantly lower computational cost as with the quantum generalized Förster theory. Larger deviations between the two theories are expected for large energy gaps as they occur in complexes with chemically different pigments.
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