Supramolecular triad and pentad composed of zinc-porphyrin(s), oxoporphyrinogen, and fullerene(s): design and electron-transfer studies

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dc.contributor Wichita State University. Department of Chemistry en_US
dc.contributor.author Schumacher, Amy Lea en_US
dc.contributor.author Sandanayaka, Atula S. D. en_US
dc.contributor.author Hill, Jonathan P. en_US
dc.contributor.author Ariga, Katsuhiko en_US
dc.contributor.author Karr, Paul A. en_US
dc.contributor.author Araki, Yasuyaki en_US
dc.contributor.author Ito, Osamu en_US
dc.contributor.author D'Souza, Francis en_US
dc.date.accessioned 2012-02-06T17:16:02Z
dc.date.available 2012-02-06T17:16:02Z
dc.date.issued 2007-01-01 en_US
dc.identifier 17385764 en_US
dc.identifier 9513783 en_US
dc.identifier.citation Chemistry (Weinheim an der Bergstrasse, Germany). 2007; 13(16): 4628-35. en_US
dc.identifier.issn 0947-6539 en_US
dc.identifier.uri http://dx.doi.org/10.1002/chem.200601854 en_US
dc.identifier.uri http://hdl.handle.net/10057/4297
dc.description Click on the DOI link below to access the article (may not be free). en_US
dc.description.abstract By adopting a "covalent-coordinate" bonding approach, novel supramolecular pentad and triad molecules composed of zinc-porphyrin(s), fullerene(s), and oxoporphyrinogen redox-/photoactive entities have been constructed, and also characterized by means of spectral and electrochemical techniques. The geometry and electronic structures of the pentad and the triad were deduced by means of DFT calculations. Free-energy calculations suggested that the photoinduced electron/energy transfer from the zinc-porphyrin (ZnP) singlet-excited state to the imidazole modified fullerene (ImC(60)) acceptor and oxoporphyrinogen (OxP) entities is feasible for both the triad and the pentad. The charge-separation rates (k(CS)) determined from picosecond time-resolved emission studies were higher for pentad (C(60)Im:ZnP)(2)-OxP than for the corresponding triad, C(60)Im:ZnP-OxP. A comparison of the k(CS) values previously reported for the covalently linked bis(zinc-porphyrin)-oxoporphyrinogen triad suggests that employing a fullerene acceptor improves the electron-transfer rates. Nanosecond transient absorption studies provide evidence for the occurrence of electron-transfer processes. Lifetimes of the radical ion pairs (tau(RIP)) are in the range of hundreds of nanoseconds, which indicates that there is charge stabilization in the supramolecular systems. en_US
dc.format.extent 4628-35 en_US
dc.language.iso eng en_US
dc.publisher John Wiley and Sons en_US
dc.relation.ispartofseries Chemistry (Weinheim an der Bergstrasse, Germany) en_US
dc.relation.ispartofseries Chemistry en_US
dc.source NLM en_US
dc.subject Research Support, Non-U.S. Gov't en_US
dc.subject Research Support, U.S. Gov't, Non-P.H.S. en_US
dc.subject.mesh Electrochemistry en_US
dc.subject.mesh Electrons en_US
dc.subject.mesh Fullerenes/chemistry en_US
dc.subject.mesh Macromolecular Substances/chemistry en_US
dc.subject.mesh Magnetic Resonance Spectroscopy/instrumentation en_US
dc.subject.mesh Models, Chemical en_US
dc.subject.mesh Molecular Structure en_US
dc.subject.mesh Photochemistry en_US
dc.subject.mesh Porphyrinogens/chemistry en_US
dc.subject.mesh Porphyrins/chemistry en_US
dc.subject.mesh Sensitivity and Specificity en_US
dc.subject.mesh Spectrometry, Fluorescence/methods en_US
dc.subject.mesh Spectrophotometry, Ultraviolet/methods en_US
dc.subject.mesh Time Factors en_US
dc.subject.mesh Zinc/chemistry en_US
dc.subject.mesh Magnetic Resonance Spectroscopy/methods en_US
dc.title Supramolecular triad and pentad composed of zinc-porphyrin(s), oxoporphyrinogen, and fullerene(s): design and electron-transfer studies en_US
dc.type Article en_US
dc.coverage.spacial Germany en_US
dc.description.version peer reviewed en_US
dc.rights.holder Copyright © 2007 WILEY-VCH Verlag GmbH & Co. en_US

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