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Excitation-wavelength-dependent, ultrafast photoinduced electron transfer in bisferrocene/BF2-chelated-azadipyrromethene/fullerene tetrads

Title
Excitation-wavelength-dependent, ultrafast photoinduced electron transfer in bisferrocene/BF2-chelated-azadipyrromethene/fullerene tetrads
Authors
Bandi V.El-Khouly M.E.Ohkubo K.Nesterov V.N.Zandler M.E.Fukuzumi S.D'Souza F.
Ewha Authors
Shunichi Fukuzumi
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2013
Journal Title
Chemistry - A European Journal
ISSN
0947-6539JCR Link
Citation
vol. 19, no. 22, pp. 7221 - 7230
Indexed
SCI; SCIE; SCOPUS WOS scopus
Abstract
Donor-acceptor distance, orientation, and photoexcitation wavelength are key factors in governing the efficiency and mechanism of electron-transfer reactions both in natural and synthetic systems. Although distance and orientation effects have been successfully demonstrated in simple donor-acceptor dyads, revealing excitation-wavelength-dependent photochemical properties demands multimodular, photosynthetic-reaction-center model compounds. Here, we successfully demonstrate donor- acceptor excitation-wavelength-dependent, ultrafast charge separation and charge recombination in newly synthesized, novel tetrads featuring bisferrocene, BF2-chelated azadipyrromethene, and fullerene entities. The tetrads synthesized using multistep synthetic procedure revealed characteristic optical, redox, and photo reactivities of the individual components and featured "closely" and "distantly" positioned donor-acceptor systems. The near-IR-emitting BF2-chelated azadipyrromethene acted as a photosensitizing electron acceptor along with fullerene, while the ferrocene entities acted as electron donors. Both tetrads revealed excitation-wavelength-dependent, photoinduced, electron-transfer events as probed by femtosecond transient absorption spectroscopy. That is, formation of the Fc+-ADP-C60 .- charge-separated state upon C60 excitation, and Fc+-ADP.--C 60 formation upon ADP excitation is demonstrated. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
DOI
10.1002/chem.201204317
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자연과학대학 > 화학·나노과학전공 > Journal papers
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