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dc.contributor.authorLim, Gary N.
dc.contributor.authorMaligaspe, Eranda
dc.contributor.authorZandler, Melvin E.
dc.contributor.authorD'Souza, Francis
dc.date.accessioned2015-01-13T03:21:23Z
dc.date.available2015-01-13T03:21:23Z
dc.date.issued2014-12-15
dc.identifier.citationLim, Gary N.; Maligaspe, Eranda; Zandler, Melvin E.; D'Souza, Francis. 2014. A Supramolecular tetrad featuring covalently linked ferrocene-zinc porphyrin-BODIPY coordinated to fullerene: a charge stabilizing, photosynthetic antenna-reaction center mimic. Chemistry - A European Journal, vol. 20:no. 51:pp 17089–17099en_US
dc.identifier.issn0947-6539
dc.identifier.otherWOS:000346056600032
dc.identifier.urihttp://dx.doi.org/10.1002/chem.201404671
dc.identifier.urihttp://hdl.handle.net/10057/11041
dc.descriptionClick on the DOI link to access the article (may not be free).en_US
dc.description.abstractA novel photosynthetic-antenna-reaction-center model compound, comprised of BF2-chelated dipyrromethene (BODIPY) as an energy-harvesting antenna, zinc porphyrin (ZnP) as the primary electron donor, ferrocene (Fc) as a hole-shifting agent, and phenylimidazole-functionalized fulleropyrrolidine (C(60)Im) as an electron acceptor, has been synthesized and characterized. Optical absorption and emission, computational structure optimization, and cyclic voltammetry studies were systematically performed to establish the role of each entity in the multistep photochemical reactions. The energy-level diagram established from optical and redox data helped identifying different photochemical events. Selective excitation of BODIPY resulted in efficient singlet energy transfer to the ZnP entity. Ultrafast electron transfer from the (ZnP)-Zn-1* (formed either as a result of singletsinglet energy transfer or direct excitation) or C-1(60)* of the coordinated fullerene resulting into the formation of the Fc-(C-60(-) Im: ZnPC+)-BODIPY radical ion pair was witnessed by femtosecond transient absorption studies. Subsequent hole migration to the ferrocene entity resulted in the Fc(+)-(C-60(+) Im: ZnP)-BODIPY radical ion pair that persisted for 7-15 ms, depending upon the solvent conditions and contributions from the triplet excited states of ZnP and ImC(60), as revealed by the nanosecond transient spectral studies. Better utilization of light energy in generating the long-lived charge-separated state with the help of the present "antenna- reaction-center" model system has been successfully demonstrated.en_US
dc.description.sponsorshipNational Science Foundation (Grant Nos. 1110942 and 1401188 to FD).en_US
dc.language.isoen_USen_US
dc.publisherWILEY-VCH Verlag GmbH & Co.en_US
dc.relation.ispartofseriesChemistry - A European Journal;v.20:no.51
dc.subjectArtificial photosynthesisen_US
dc.subjectBODIPYen_US
dc.subjectCharge stabilizationen_US
dc.subjectFerroceneen_US
dc.subjectFullerenesen_US
dc.subjectElectron transferen_US
dc.subjectZinc porphyrinen_US
dc.titleA Supramolecular tetrad featuring covalently linked ferrocene-zinc porphyrin-BODIPY coordinated to fullerene: a charge stabilizing, photosynthetic antenna-reaction center mimicen_US
dc.typeArticleen_US
dc.rights.holderCopyright 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim


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