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Exciton dynamics in the chlorosomal antenna of the green bacterium Chloroflexus aurantiacus: experimental and theoretical studies of femtosecond pump-probe spectra

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Abstract

Femtosecond absorption difference spectra were measured for chlorosomes isolated from the green bacterium Chloroflexus aurantiacus at room temperature. Using the relative difference absorption of the oligomeric BChl c and monomeric BChl a bands, the size of a unit BChl c aggregate as well as the exciton coherence size were estimated for the chlorosomal BChl c antenna under study. A quantitative fit of the data was obtained within the framework of the exciton model proposed before [Fetisova et al. (1996) Biophys J 71: 995–1010]. The size of the antenna unit was found to be 24 exciton-coupled BChl c molecules. The anomalously high bleaching value of the oligomeric B740 band with respect to the monomeric B795 band provided the direct evidence for a high degree of exciton delocalization in the chlorosomal B740 BChl c antenna. The effective delocalization size of individual exciton wavefunctions (the thermally averaged inverse participation ratio) in the chlorosomal BChl c antenna is 9.5, whereas the steady-state wavepacket corresponds to the coherence size (the inverse participation ratio of the density matrix) of 7.4 at room temperature.

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Authors and Affiliations

  1. A. N. Belozersky Institute of Physico-Chemical Biology, Moscow State University, Moscow, 119899, Russia

    Andrey Yakovlev, Vladimir Novoderezhkin, Alexandra Taisova & Zoya Fetisova

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  1. Andrey Yakovlev
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  2. Vladimir Novoderezhkin
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  3. Alexandra Taisova
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  4. Zoya Fetisova
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Correspondence to Zoya Fetisova.

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Yakovlev, A., Novoderezhkin, V., Taisova, A. et al. Exciton dynamics in the chlorosomal antenna of the green bacterium Chloroflexus aurantiacus: experimental and theoretical studies of femtosecond pump-probe spectra. Photosynthesis Research 71, 19–32 (2002). https://doi.org/10.1023/A:1014995328869

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