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JOURNAL ARTICLE
RESEARCH SUPPORT, NON-U.S. GOV'T
Mediating Reductive Charge Shift Reactions in Electron Transport Chains.
Journal of the American Chemical Society 2017 December 7
We report the synthesis of a full-fledged family of covalent electron donor-acceptor1 -acceptor2 conjugates and their charge-transfer characterization by means of advanced photophysical assays. By virtue of variable excited state energies and electron donor strengths, either Zn(II)Porphyrins or Zn(II)Phthalocyanines were linked to different electron-transport chains featuring pairs of electron accepting fullerenes, that is, C60 and C70 . In this way, a fine-tuned redox gradient is established to power a unidirectional, long-range charge transport from the excited-state electron donor via a transient C60 •- toward C70 •- . This strategy helps minimize energy losses in the reductive, short-range charge shift from C60 to C70 . At the forefront of our investigations are excited-state dynamics deduced from femtosecond transient absorption spectroscopic measurements and subsequent computational deconvolution of the transient absorption spectra. These provide evidence for cascades of short-range charge-transfer processes, including reductive charge shift reactions between the two electron-accepting fullerenes, and for kinetics that are influenced by the nature and length of the respective spacer. Of key importance is the postulate of a mediating state in the charge-shift reaction at weak electronic couplings. Our results point to an intimate relationship between triplet-triplet energy transfer and charge transfer.
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