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- W2912246201 abstract "Redox-active proteins covalently modified with photosensitizers have served as important model systems for elucidation of kinetic principles controlling biological electron transfer. To date, the fastest rates observed in these systems were ∼10ns and involved donor acceptor (DA) distances of >0.8nm. This leaves a significant gap in rates and distances for charge transfer rates occurring in Nature but poorly accessible in experimental studies. To this end, we developed a series of 22 cysteine mutants of PpcA, a 3-heme cytochrome from Geobacter sulfurreducens. Due to its relatively small size (71 amino acids) we expected to obtain a number of mutants with DA distance of 0.4-0.5nm. These proteins were successfully expressed in E.coli and isolated for covalent labeling with Ru(bpy)2(bpy-Br). With time-resolved nanosecond and ultrafast transient absorbance spectroscopy we have identified 6 constructs with apparent photo-induced charge transfer time constants of 20 ps or faster, including 2 constructs with 1-2 ps time constants. The is a significant result as up to this point only natural photosynthetic systems demonstrated such a fast initial charge separation, while all artificial covalent biohybrid constructs exhibited charge transfer rates 3 or more orders of magnitude slower. To understand molecular principles responsible for such a dramatic acceleration of electron transfer rates, we used small- and wide angle X-ray scattering and currently attempting to obtain X-ray crystallographic and NMR structures of ultrafast constructs. Finally, we performed triplicate 250-300 ns all-atom molecular dynamics simulations of all 6 ultrafast constructs. Based on the obtained results we conclude that that photo-induced ultrafast charge transfer requires van der Waals contact between heme vinyl groups and photosensitizers while contacts with propionates or a small number of covalent bonds between the donors and acceptors play much less significant role." @default.
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- W2912246201 date "2019-02-01" @default.
- W2912246201 modified "2023-09-30" @default.
- W2912246201 title "Mimicking Natural Photosynthesis Ultrafast Charge Transfer in PpcA-Photosensitizer Complexes" @default.
- W2912246201 doi "https://doi.org/10.1016/j.bpj.2018.11.2252" @default.
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