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dc.contributor.authorD'Souza, Francis
dc.contributor.authorDas, Sushanta K.
dc.contributor.authorSandanayaka, Atula S. D.
dc.contributor.authorSubbaiyan, Navaneetha K.
dc.contributor.authorGollapalli, Deviprasad R.
dc.contributor.authorZandler, Melvin E.
dc.contributor.authorWakahara, Takatsugu
dc.contributor.authorIto, Osamu
dc.date.accessioned2012-06-01T20:30:59Z
dc.date.available2012-06-01T20:30:59Z
dc.date.issued2012-12-14
dc.identifier.citationD'Souza F, SK Das, AS Sandanayaka, NK Subbaiyan, DR Gollapalli, ME Zandler, T Wakahara, and O Ito. 2012. "Photoinduced charge separation in three-layer supramolecular nanohybrids: fullerene-porphyrin-SWCNT.". Physical Chemistry Chemical Physics : PCCP. 14 (8): 2940-50.en_US
dc.identifier.issn1463-9076
dc.identifier.issn1463-9084
dc.identifier.urihttp://hdl.handle.net/10057/5113
dc.identifier.urihttp://dx.doi.org/10.1039/c2cp23643e
dc.descriptionClick on the DOI link to access the article (may not be free).en_US
dc.description.abstractPhotoinduced charge separation processes of three-layer supramolecular hybrids, fullerene-porphyrin-SWCNT, which are constructed from semiconducting (7,6)- and (6,5)-enriched SWCNTs and self-assembled via pi-pi interacting long alkyl chain substituted porphyrins (tetrakis(4-dodecyloxyphenyl)porphyrins; abbreviated as MP(alkyl)(4)) (M = Zn and H-2), to which imidazole functionalized fullerene[60] (C(60)Im) is coordinated, have been investigated in organic solvents. The intermolecular alkyl-pi and pi-pi interactions between the MP (alkyl)(4) and SWCNTs, in addition, coordination between C(60)Im and Zn ion in the porphyrin cavity are visualized using DFT calculations at the B3LYP/3-21G(*) level, predicting donor-acceptor interactions between them in the ground and excited states. The donor-acceptor nanohybrids thus formed are characterized by TEM imaging, steady-state absorption and fluorescence spectra. The time-resolved fluorescence studies of MP(alkyl)(4) in two-layered nanohybrids (MP(alkyl)(4)/SWCNT) revealed efficient quenching of the singlet excited states of MP(alkyl)(4) ((MP)-M-1*(alkyl)(4)) with the rate constants of charge separation (k(CS)) in the range of (1-9) x 10(9) s(-1). A nanosecond transient absorption technique confirmed the electron transfer products, MP center dot+(alkyl)(4)/SWCNT center dot- and/or MP center dot-(alkyl)(4)/SWCNT center dot+ for the two-layer nanohybrids. Upon further coordination of C(60)Im to ZnP, acceleration of charge separation via (ZnP)-Zn-1* in C(60)Im -> ZnP(alkyl)(4)/SWCNT is observed to form C(60)(center dot-)Im -> ZnP center dot+(alkyl)(4)/SWCNT and C(60)(center dot-)Im -> ZnP(alkyl)(4)/SWCNT center dot+ charge separated states as supported by the transient absorption spectra. These characteristic absorptions decay with rate constants due to charge recombination (k(CR)) in the range of (6-10) x 10(6) s(-1), corresponding to the lifetimes of the radical ion-pairs of 100-170 ns. The electro! n transfer in the nanohybrids has further been utilized for light-to-electricity conversion by the construction of proof-of-concept photoelectrochemical solar cells.en_US
dc.description.sponsorshipThis work was financially supported by the National Science Foundation (Grant No. 1110942 to FD). The authors would like to thank Prof. H. Murata of JAIST for support
dc.language.isoen_USen_US
dc.publisherRoyal Society of Chemistryen_US
dc.relation.ispartofseriesPhysical Chemistry Chemical Physics: PCCP;2012 :, v.14, no.8
dc.titlePhotoinduced charge separation in three-layer supramolecular nanohybrids: fullerene-porphyrin-SWCNTen_US
dc.typeArticleen_US
dc.description.versionPeer reviewed


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