The Role of Exciton Delocalization in the Major Photosynthetic Light-Harvesting Antenna of Plants
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In the major peripheral plant light-harvesting complex LHCII, excitation energy is transferred between chlorophylls along an energetic cascade before it is transmitted further into the photosynthetic assembly to be converted into chemical energy. The efficiency of these energy transfer processes involves a complicated interplay of pigment-protein structural reorganization and protein dynamic disorder, and the system must stay robust within the fluctuating protein environment. The final, lowest energy site has been proposed to exist within a trimeric excitonically coupled chlorophyll (Chl) cluster, comprising Chls a610-a611-a612. We studied an LHCII monomer with a site-specific mutation resulting in the loss of Chls a611and a612, and find that this mutant exhibits two predominant overlapping fluorescence bands. From a combination of bulk measurements, single-molecule fluorescence characterization, and modeling, we propose the two fluorescence bands originate from differing conditions of exciton delocalization and localization realized in the mutant. Disruption of the excitonically coupled terminal emitter Chl trimer results in an increased sensitivity of the excited state energy landscape to the disorder induced by the protein conformations. Consequently, the mutant demonstrates a loss of energy transfer efficiency. On the contrary, in the wild-type complex, the strong resonance coupling and correspondingly high degree of excitation delocalization within the Chls a610-a611-a612 cluster dampens the influence of the environment and ensures optimal communication with neighboring pigments. These results indicate that the terminal emitter trimer is thus an essential design principle for maintaining the efficient light-harvesting function of LHCII in the presence of protein disorder.
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Static disorder also strongly affects the fate of an excitation in a light-harvesting complex by changing the probability of the excitation to be trapped in an energy sink or by pigment clusters that are not neighbouring other complexes in the photosystem.
“Static disorder also strongly affects the fate of an excitation in a light-harvesting complex by changing the probability of the excitation to be trapped in an energy sink [63,64] or by pigment clusters that are not neighbouring other complexes in the photosystem [65].”
From The future of quantum biology (2018) · cites this paper as [65]
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- Authors
- Ramanan, C., Gruber, J. M., Malý, P., Negretti, M., Novoderezhkin, V., Krüger, T. P. J., Mančal, T., Croce, R., & van Grondelle, R.
- Affiliations
- Vrije Universiteit Amsterdam (NL)
- Charles University (CZ)
- Lomonosov Moscow State University (RU)
- University of Pretoria (ZA)
- Corresponding author
- Ramanan, Charusheela
- ORCID
- Venue
- Biophysical Journal
- Publisher
- Elsevier BV
- Published
- 2015-03
- Volume
- 108
- Issue
- 5
- Pages
- 1047-1056
- ISSN
- 0006-3495 (ISSN-L)
- PMC
- PMC4375621
- OpenAlex
- W1980563015
- Cited by
- 28
- References
- 57
- Citations by year
- 2025: 1 · 2024: 1 · 2023: 1 · 2022: 5 · 2021: 2 · 2020: 7 · 2019: 2 · 2018: 3 · 2017: 3 · 2015: 3
- FWCI
- 1.52
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Licence
- Locations
- Biophysical Journal (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- VU Research Portal (publishedVersion, other-oa)
- MPG.PuRe (Max Planck Society) (submittedVersion)
- UpSpace Institutional Repository (University of Pretoria) (submittedVersion)
- VU Research Portal (submittedVersion, other-oa)
- Data Archiving and Networked Services (DANS) (submittedVersion, other-oa)
- Funders
- Nederlandse Organisatie voor Wetenschappelijk Onderzoek (700.58.305, 040.11.428, 040.11.423)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Keywords
- light-harvesting complex II, light-harvesting complexes, exciton delocalization, exciton localization, energy transfer efficiency, protein disorder, site-specific mutations, single-molecule fluorescence, resonant coupling, photosynthetic antenna
- MeSH terms
- Fluorescence, Mutation, Arabidopsis, Arabidopsis Proteins, Light-Harvesting Protein Complexes, Protein Multimerization
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