Abstract
The energy and charge-transfer processes in photosystem I (PS I) complexes isolated from cyanobacteria Thermosynechococcus elongatus and Synechocystis sp. PCC 6803 were investigated by pump-to-probe femtosecond spectroscopy. The formation of charge-transfer (CT) states in excitonically coupled chlorophyll a complexes (exciplexes) was monitored by measuring the electrochromic shift of β-carotene in the spectral range 500–510 nm. The excitation of high-energy chlorophyll in light-harvesting antenna of both species was not accompanied by immediate appearance of an electrochromic shift. In PS I from T. elongatus, the excitation of long-wavelength chlorophyll (LWC) caused a pronounced electrochromic effect at 502 nm assigned to the appearance of CT states of chlorophyll exciplexes. The formation of ion-radical pair P700+A1− at 40 ps was limited by energy transfer from LWC to the primary donor P700 and accompanied by carotenoid bleach at 498 nm. In PS I from Synechocystis 6803, the excitation at 720 nm produced an immediate bidentate bleach at 690/704 nm and synchronous carotenoid response at 508 nm. The bidentate bleach was assigned to the formation of primary ion-radical state PB+Chl2B−, where negative charge is localized predominantly at the accessory chlorophyll molecule in the branch B, Chl2B. The following decrease of carotenoid signal at ~ 5 ps was ascribed to electron transfer to the more distant molecule Chl3B. The reduction of phylloquinone in the sites A1A and A1B was accompanied by a synchronous blue-shift of the carotenoid response to 498 nm, pointing to fast redistribution of unpaired electron between two branches in favor of the state PB+A1A−.
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Acknowledgements
This work was supported by Russian Foundation for Basic Research Grants 17-04-01717, 17-00-00201, 17-00-00209 and 17-00-00207 (complex project 17-00-00218) and by the N. N. Semenov Federal Research Center for Chemical Physics, Russian Academy of Sciences State task AAAA-A19-119012890064-7. Also investigations were performed using the facilities of N. N. Semenov Federal Research Center for Chemical Physics, Russian Academy of Sciences CCE (No. 506694).
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Cherepanov, D.A., Shelaev, I.V., Gostev, F.E. et al. Generation of ion-radical chlorophyll states in the light-harvesting antenna and the reaction center of cyanobacterial photosystem I. Photosynth Res 146, 55–73 (2020). https://doi.org/10.1007/s11120-020-00731-0
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DOI: https://doi.org/10.1007/s11120-020-00731-0