ArticleThe journal of physical chemistry letters2023
Origin of Low-Lying Red States in the Lhca4 Light-Harvesting Complex of Photosystem I.
Article in The journal of physical chemistry letters, 2023. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 16 papers.
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16 citing papers in PubMed, 25 citations in OpenAlex.
- Article
- Structural and spectral adaptation of the seagrass Posidonia oceanica photosystem I to seabed light.Nature communications · 2026Article
- Far-red chlorophyll d clusters extend photosystem I absorption toward the red limit.Science advances · 2026Article
- Isolating the Vibrational Spectra of the Red Chlorophylls in Photosystem I with Multispectral Two-Dimensional Spectroscopy.The journal of physical chemistry letters · 2026Article
- A design principle for tuning far-red absorption of chlorophyll a in light-harvesting complexes.Communications chemistry · 2026Article
- Cryo-EM structure of a photosystem I supercomplex from Euglena gracilis containing pentameric LHCE and dimeric LHCII.Nature communications · 2026Article
- Photosynthesis under far-red light-evolutionary adaptations and bioengineering of light-harvesting complexes.FEBS letters · 2026Review
- Exciton Delocalization Promotes Far-Red Absorption in a Tetrameric ChlorophyllJournal of the American Chemical Society · 2025Article
- Structural determinants for red-shifted absorption in higher-plants Photosystem I.The New phytologist · 2025Article
- Eustigmatophyte model of red-shifted chlorophyll a absorption in light-harvesting complexes.Communications biology · 2024Article
- Perspectives on improving photosynthesis to increase crop yield.The Plant cell · 2024Review
- Structure of the red-shifted Fittonia albivenis photosystem I.Nature communications · 2024Article
- Excitation landscape of the CP43 photosynthetic antenna complex from multiscale simulations.Chemical science · 2024Article
- Coloring Outside the Lines: Exploiting Pigment-Protein Synergy for Far-Red Absorption in Plant Light-Harvesting Complexes.Journal of the American Chemical Society · 2024Article
- Integrated eQTL mapping approach reveals genomic regions regulating candidate genes of theFrontiers in plant science · 2024Article
- Environment-dependent chlorophyll-chlorophyll charge transfer states in Lhca4 pigment-protein complex.Frontiers in plant science · 2024Article
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Authors and funding
6 authors at 2 institutions in 2 countries.
Funding
No grant is acknowledged in the PubMed record.
Abstract
The antenna complexes of Photosystem I present low-lying states visible as red-shifted and broadened absorption and fluorescence bands. Among these, Lhca4 has the most evident features of these "red" states, with a fluorescence band shifted by more than 25 nm from typical LHC emission. This signal arises from a mixing of exciton and charge-transfer (CT) states within the excitonically coupled a603-a609 chlorophyll (Chl) dimer. Here we combine molecular dynamics, multiscale quantum chemical calculations, and spectral simulations to uncover the molecular mechanism for the formation and tuning of exciton-CT interactions in Lhca4. We show that the coupling between exciton and CT states is extremely sensitive to tiny variations in the Chl dimer arrangement, explaining both the red-shifted bands and the switch between conformations with blue and red emission observed in single-molecule spectroscopy. Finally, we show that mutating the axial ligand of a603 diminishes the exciton-CT coupling, removing any red-state fingerprint.
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