Show simple item record

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.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.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.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.description.versionPeer reviewed

Files in this item


There are no files associated with this item.

This item appears in the following Collection(s)

Show simple item record