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Femtosecond Exciton Relaxation in Chlorosomes of the Photosynthetic Green Bacterium Chloroflexus aurantiacus

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Abstract

Process of photosynthesis in the green bacteria Chloroflexus (Cfx.) aurantiacus starts from absorption of light by chlorosomes, peripheral antennas consisting of thousands of bacteriochlorophyll c (BChl c) molecules combined into oligomeric structures. In this case, the excited states are formed in BChl c, energy of which migrates along the chlorosome towards the baseplate and further to the reaction center, where the primary charge separation occurs. Energy migration is accompanied by non-radiative electronic transitions between the numerous exciton states, that is, exciton relaxation. In this work, we studied dynamics of the exciton relaxation in Cfx. aurantiacus chlorosomes using differential femtosecond spectroscopy at cryogenic temperature (80 K). Chlorosomes were excited by 20-fs light pulses at wavelengths in the range from 660 to 750 nm, and differential (light-dark) absorption kinetics were measured at a wavelength of 755 nm. Mathematical analysis of the obtained data revealed kinetic components with characteristic times of 140, 220, and 320 fs, which are responsible for exciton relaxation. As the excitation wavelength decreased, the number and relative contribution of these components increased. Theoretical modelling of the obtained data was carried out based of the cylindrical model of BChl c. Nonradiative transitions between the groups of exciton bands were described by a system of kinetic equations. The model that takes into account energy and structural disorder of chlorosomes turned out to be the most adequate.

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Abbreviations

BChl:

bacteriochlorophyll

ΔA :

absorption difference (light-dark)

τ1-6 :

characteristic time of the kinetic components

λex :

excitation wavelength

λprobe :

probe wavelength

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Acknowledgments

The authors express their deep gratitude to the late Academician V.A. Shuvalov for general support and constant attention to their work.

Funding

The study was financially supported by the State Budget Project No. AAAA-A17-117120540070-0 (“Photobiophysics of solar energy conversion in living systems”).

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Authors and Affiliations

  1. Belozersky Institute of Physico-Chemical Biology, Lomonosov Moscow State University, 119992, Moscow, Russia

    Andrei G. Yakovlev, Alexandra S. Taisova & Zoya G. Fetisova

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  1. Andrei G. Yakovlev
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  2. Alexandra S. Taisova
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  3. Zoya G. Fetisova
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Contributions

Z.G.F. – supervision of the work, discussion of the results; A.G.Y. – supervision, conducting experiments and calculations, discussion of the results, writing an article; A.S.T. – cultivation of bacteria, preparing samples, writing the article.

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Correspondence to Andrei G. Yakovlev.

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The authors declare no conflicts of interest in financial or any other sphere. This article does not contain description of studies involving humans or animals performed by any of the authors.

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Yakovlev, A.G., Taisova, A.S. & Fetisova, Z.G. Femtosecond Exciton Relaxation in Chlorosomes of the Photosynthetic Green Bacterium Chloroflexus aurantiacus. Biochemistry Moscow 88, 704–715 (2023). https://doi.org/10.1134/S0006297923050139

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