ArticleThe journal of physical chemistry. B2020
Dynamic Disorder Drives Exciton Transfer in Tubular Chlorosomal Assemblies.
Article in The journal of physical chemistry. B, 2020. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 13 papers.
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13 citing papers in PubMed, 28 citations in OpenAlex.
- Conformational Dynamics of BacteriochlorophyllThe journal of physical chemistry. B · 2025Article
- Self-aggregation of 13Photochemical & photobiological sciences : Official journal of the European Photochemistry Association and the European Society for Photobiology · 2024Article
- Contrasting packing modes for tubular assemblies in chlorosomes.Photosynthesis research · 2024Article
- Observation of Dark States in Two-Dimensional Electronic Spectra of Chlorosomes.The journal of physical chemistry. B · 2024Article
- Photon Energy-Dependent Ultrafast Exciton Transfer in Chlorosomes ofThe journal of physical chemistry. B · 2023Article
- Ultrafast Anisotropy Decay Reveals Structure and Energy Transfer in Supramolecular Aggregates.The journal of physical chemistry. B · 2023Article
- Manifestation of Hydrogen Bonding and Exciton Delocalization on the Absorption and Two-Dimensional Electronic Spectra of Chlorosomes.The journal of physical chemistry. B · 2023Article
- Static Disorder has Dynamic Impact on Energy Transport in Biomimetic Light-Harvesting Complexes.The journal of physical chemistry. B · 2022Article
- The role of chirality and plastic crystallinity in the optical and mechanical properties of chlorosomes.iScience · 2022Article
- Limitations of Linear Dichroism Spectroscopy for Elucidating Structural Issues of Light-Harvesting Aggregates in Chlorosomes.Molecules (Basel, Switzerland) · 2021Article
- Tuning the Proton-Coupled Electron-Transfer Rate by Ligand Modification in Catalyst-Dye Supramolecular Complexes for Photocatalytic Water Splitting.ChemSusChem · 2021Article
- Molecular versus Excitonic Disorder in Individual Artificial Light-Harvesting Systems.Journal of the American Chemical Society · 2020Article
- Multiscale modeling of molecular structure and optical properties of complex supramolecular aggregates.Chemical science · 2020Article
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Authors and funding
4 authors at 1 institution in 1 country.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Chlorosomes stand out for their highly efficient excitation energy transfer (EET) in extreme low light conditions. Yet, little is known about the EET when a chlorosome is excited to a pure state that is an eigenstate of the exciton Hamiltonian. In this work, we consider the dynamic disorder in the intermolecular electronic coupling explicitly by calculating the electronic coupling terms in the Hamiltonian using nuclear coordinates that are taken from molecular dynamics simulation trajectories. We show that this dynamic disorder is capable of driving the evolution of the exciton, being a stationary state of the initial Hamiltonian. In particular, long-distance excitation energy transfer between domains of high exciton population and oscillatory behavior of the population in the site basis are observed, in line with two-dimensional electronic spectroscopy studies. We also found that in the high exciton population domains, their population variation is correlated with their overall coupling strength. Analysis in a reference state basis shows that such dynamic disorder, originating from thermal energy, creates a fluctuating landscape for the exciton and promotes the EET process. We propose such dynamic disorder as an important microscopic origin for the high efficient EET widely observed in different types of chlorosomes, bioinspired tubular aggregates, or other light-harvesting complexes.
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