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Excitation energy transfer dynamics and excited-state structure in chlorosomes of Chlorobium phaeobacteroides

AutorPsencik, Jakub; Ma, Ying-Zhong; Arellano, Juan B. ; Hála, Jan; Gillbro, Tomas
Palabras claveChlorosomes
Chlorobium phaeobacteroides
Energy transfer
Bacteriochlorophyll e
Bacteriochlorophyll a
Femtosecond transient absorption
Fecha de publicaciónfeb-2003
EditorRockefeller University Press
CitaciónBiophysical Journal. Volume 84 February 2003 1161-1179
ResumenThe excited-state relaxation within bacteriochlorophyll (BChl) e and a in chlorosomes of Chlorobium phaeobacteroides has been studied by femtosecond transient absorption spectroscopy at room temperature. Singlet-singlet annihilation was observed to strongly influence both the isotropic and anisotropic decays. Pump intensities in the order of 10(11) photons x pulse(-1) x cm(-2) were required to obtain annihilation-free conditions. The most important consequence of applied very low excitation doses is an observation of a subpicosecond process within the BChl e manifold (similar to200-500 fs), manifesting itself as a rise in the red part of the Q(y) absorption band of the BChl e aggregates. The subsequent decay of the kinetics measured in the BChl e region and the corresponding rise in the baseplate BChl a is not single-exponential, and at least two components are necessary to fit the data, corresponding to several BChl e-->BChl a transfer steps. Under annihilation-free conditions, the anisotropic kinetics show a generally slow decay within the BChl e band (10-20 ps) whereas it decays more rapidly in the BChl a region (similar to1 ps). Analysis of the experimental data gives a detailed picture of the overall time evolution of the energy relaxation and energy transfer processes within the chlorosome. The results are interpreted within an exciton model based on the proposed structure.
Versión del editorhttp://www.pubmedcentral.nih.gov/articlerender.fcgi?tool=pubmed&pubmedid=12547796
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