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Fluorescence Spectral Dynamics of Single LHCII Trimers

Single-molecule spectroscopy was employed to elucidate the fluorescence spectral heterogeneity and dynamics of individual, immobilized trimeric complexes of the main light-harvesting complex of plants in solution near room temperature. Rapid reversible spectral shifts between various emitting states, each of which was quasi-stable for seconds to tens of seconds, were observed for a fraction of the complexes. Most deviating states were characterized by the appearance of an additional, red-shifted emission band. Reversible shifts of up to 75 nm were detected. By combining modified Redfield theory with a disordered exciton model, fluorescence spectra with peaks between 670 nm and 705 nm could be explained by changes in the realization of the static disorder of the pigment-site energies. Spectral bands beyond this wavelength window suggest the presence of special protein conformations. We attribute the large red shifts to the mixing of an excitonic state with a charge-transfer state in two or more strongly coupled chlorophylls. Spectral bluing is explained by the formation of an energy trap before excitation energy equilibration is completed.
- Free University of Amsterdam Pure VU Amsterdam Netherlands
- Lomonosov Moscow State University Russian Federation
- Vrije Universiteit Amsterdam Netherlands
- Vrije Universiteit Brussel Belgium
Spectrometry, Fluorescence, Energy Transfer, Biophysics, Light-Harvesting Protein Complexes, Temperature, SDG 7 - Affordable and Clean Energy, Protein Multimerization, Protein Structure, Quaternary
Spectrometry, Fluorescence, Energy Transfer, Biophysics, Light-Harvesting Protein Complexes, Temperature, SDG 7 - Affordable and Clean Energy, Protein Multimerization, Protein Structure, Quaternary
citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).145 popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.Top 10% influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).Top 10% impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.Top 1%
