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dc.contributorWichita State University. Department of Chemistryen_US
dc.contributor.authorD'Souza, Francisen_US
dc.contributor.authorChitta, Raghuen_US
dc.contributor.authorSandanayaka, Atula S. D.en_US
dc.contributor.authorSubbaiyan, Navaneetha K.en_US
dc.contributor.authorD'Souza, Lawrenceen_US
dc.contributor.authorAraki, Yasuyakien_US
dc.contributor.authorIto, Osamuen_US
dc.identifier.citationJournal of the American Chemical Society. 2007 Dec 26; 129(51): 15865-71.en_US
dc.descriptionClick on the DOI link below to access the article (may not be free).en_US
dc.description.abstractPhotoinduced electron transfer in a self-assembled single-wall carbon nanotube (SWNT)-fullerene(C60) hybrid with SWNT acting as an electron donor and fullerene as an electron acceptor has been successfully demonstrated. Toward this, first, SWNTs were noncovalently functionalized using alkyl ammonium functionalized pyrene (Pyr-NH3+) to form SWNT/Pyr-NH3+ hybrids. The alkyl ammonium entity of SWNT/Pyr-NH3+ hybrids was further utilized to complex with benzo-18-crown-6 functionalized fullerene, crown-C60, via ammonium-crown ether interactions to yield SWNT/Pyr-NH3+/crown-C60 nanohybrids. The nanohybrids were isolated and characterized by TEM, UV-visible-near IR, and electrochemical methods. Free-energy calculations suggested possibility of electron transfer from the carbon nanotube to the singlet excited fullerene in the SWNT/Pyr-NH3+/crown-C60 nanohybrids. Accordingly, steady-state and time-resolved fluorescence studies revealed efficient quenching of the singlet excited-state of C60 in the nanohybrids. Further studies involving nanosecond transient absorption studies confirmed electron transfer to be the quenching mechanism, in which the electron-transfer product, fullerene anion radical, was possible to spectrally characterize. The rates of charge separation, kCS, and charge recombination, kCR, were found to be 3.46 x 10(9) and 1.04 x 10(7) s-1, respectively. The calculated lifetime of the radical ion-pair was found to be over 100 ns, suggesting charge stabilization in the novel supramolecular nanohybrids. The present nanohybrids were further utilized to reduce hexyl-viologen dication (HV2+) and a sacrificial electron donor, 1-benzyl-1,4-dihydronicotinamide, in an electron-pooling experiment, offering additional proof for the occurrence of photoinduced charge-separation and potential utilization of these materials in light-energy harvesting applications.en_US
dc.publisherAmerican Chemical Societyen_US
dc.relation.ispartofseriesJournal of the American Chemical Societyen_US
dc.relation.ispartofseriesJ. Am. Chem. Soc.en_US
dc.titleSupramolecular carbon nanotube-fullerene donor-acceptor hybrids for photoinduced electron transferen_US
dc.coverage.spacialUnited Statesen_US
dc.description.versionpeer revieweden_US
dc.rights.holderCopyright © 2007 American Chemical Societyen_US

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