ArticleJournal of the American Chemical Society2013
Photosystem II does not possess a simple excitation energy funnel: time-resolved fluorescence spectroscopy meets theory.
Article in Journal of the American Chemical Society, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 48 papers.
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48 citing papers in PubMed, 136 citations in OpenAlex.
- Tuning the F695 fluorescent state in photosystem II using site-directed mutagenesis in Synechocystis sp. PCC 6803.Photosynthesis research · 2026Article
- Photosynthesis under far-red light-evolutionary adaptations and bioengineering of light-harvesting complexes.FEBS letters · 2026Review
- Revisiting the QPhotosynthesis research · 2025Review
- Microscopic basis of reaction center modulation in PsbA variants of photosystem II.Proceedings of the National Academy of Sciences of the United States of America · 2025Article
- Network analysis with quantum dynamics clarifies why photosystem II exploits both chlorophyll a and b.Science advances · 2025Article
- NIR Luminescence from Deep-Level Traps in CsPbBrThe journal of physical chemistry letters · 2025Article
- Entropy is an important design principle in the photosystem II supercomplex.Proceedings of the National Academy of Sciences of the United States of America · 2025Article
- Application of the Time-Domain Multichromophoric Fluorescence Resonant Energy Transfer Method in the NISE Programme.Journal of chemical theory and computation · 2025Article
- Design principles for energy transfer in the photosystem II supercomplex from kinetic transition networks.Nature communications · 2024Article
- Bidirectional Energy Flow in the Photosystem II Supercomplex.The journal of physical chemistry. B · 2024Article
- Protein Effects on the Excitation Energies and Exciton Dynamics of the CP24 Antenna Complex.The journal of physical chemistry. B · 2024Article
- Excitation landscape of the CP43 photosynthetic antenna complex from multiscale simulations.Chemical science · 2024Article
- Inter-subunit energy transfer processes in a minimal plant photosystem II supercomplex.Science advances · 2024Article
- Article
- Effects of lipids on the rate-limiting steps in the dark-to-light transition of Photosystem II core complex ofFrontiers in plant science · 2024Article
- Reinvestigation on primary processes of PSII-dimer from Thermosynechococcus vulcanus by femtosecond pump-probe spectroscopy.Photosynthesis research · 2024Article
- Letter to the Editor.Photosynthetica · 2024Article
- Reaction Center Excitation in Photosystem II: From Multiscale Modeling to Functional Principles.Accounts of chemical research · 2023Article
- Charge separation in the photosystem II reaction center resolved by multispectral two-dimensional electronic spectroscopy.Science advances · 2023Article
- Thermal site energy fluctuations in photosystem I: new insights from MD/QM/MM calculations.Chemical science · 2023Article
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5 authors at 3 institutions in 2 countries.
Funding
Abstract
The experimentally obtained time-resolved fluorescence spectra of photosystem II (PS II) core complexes, purified from a thermophilic cyanobacterium Thermosynechococcus vulcanus, at 5-180 K are compared with simulations. Dynamic localization effects of excitons are treated implicitly by introducing exciton domains of strongly coupled pigments. Exciton relaxations within a domain and exciton transfers between domains are treated on the basis of Redfield theory and generalized Förster theory, respectively. The excitonic couplings between the pigments are calculated by a quantum chemical/electrostatic method (Poisson-TrEsp). Starting with previously published values, a refined set of site energies of the pigments is obtained through optimization cycles of the fits of stationary optical spectra of PS II. Satisfactorily agreement between the experimental and simulated spectra is obtained for the absorption spectrum including its temperature dependence and the linear dichroism spectrum of PS II core complexes (PS II-CC). Furthermore, the refined site energies well reproduce the temperature dependence of the time-resolved fluorescence spectrum of PS II-CC, which is characterized by the emergence of a 695 nm fluorescence peak upon cooling down to 77 K and the decrease of its relative intensity upon further cooling below 77 K. The blue shift of the fluorescence band upon cooling below 77 K is explained by the existence of two red-shifted chlorophyll pools emitting at around 685 and 695 nm. The former pool is assigned to Chl45 or Chl43 in CP43 (Chl numbering according to the nomenclature of Loll et al. Nature2005, 438, 1040) while the latter is assigned to Chl29 in CP47. The 695 nm emitting chlorophyll is suggested to attract excitations from the peripheral light-harvesting complexes and might also be involved in photoprotection.
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