We investigated the fluorescence kinetics of LH2 complexes from Marichromatium purpuratum, the cryo-EM structure of which has been recently elucidated with 2.4 Å resolution. The experiments have been carried out as a function of the excitation density by varying both the excitation fluence and the repetition rate of the laser excitation. Instead of the usual multiexponential fitting procedure, we applied the less common phasor formalism for evaluating the transients because this allows for a model-free analysis of the data without a priori knowledge about the number of processes that contribute to a particular decay. For the various excitation conditions, this analysis reproduces consistently three lifetime components with decay times below 100 ps, 500 ps, and 730 ps, which were associated with the quenched state, singlet-triplet annihilation, and fluorescence decay, respectively. Moreover, it reveals that the number of decay components that contribute to the transients depends on whether the excitation wavelength is in resonance with the B800 BChl a molecules or with the carotenoids. Based on the mutual arrangement of the chromophores in their binding pockets, this leads us to conclude that the energy transfer pathways within the LH2 complex of this species differ significantly from each other for exciting either the B800 BChl molecules or the carotenoids. Finally, we speculate whether the illumination with strong laser light converts the LH2 complexes studied here into a quenched conformation that might be related to the development of the non-photochemical quenching mechanism that occurs in higher plants.

Bavarian Polymer Institute University of Bayreuth Universitätsstr 30 D 95440 Bayreuth Germany

Bayreuth Institute for Macromolecular Research University of Bayreuth Universitätsstr 30 D 95440 Bayreuth Germany

Laboratory of Anoxygenic Phototrophs Institute of Microbiology Czech Academy of Sciences 379 81 Třeboň Czech Republic

School of Biosciences University of Sheffield Sheffield S10 2TN U K

School of Infection and Immunity Glasgow University Glasgow G12 8TA U K

School of Molecular Biosciences Glasgow University Glasgow G12 8QQ U K

Spectroscopy of Soft Matter University of Bayreuth Universitätsstr 30 D 95440 Bayreuth Germany

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