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Photosynthetic antenna-reaction center mimicry: sequential energy- and electron transfer in a self-assembled supramolecular triad composed of boron dipyrrin, zinc porphyrin and fullerene

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dc.contributor Wichita State University. Department of Chemistry en_US
dc.contributor.author Maligaspe, Eranda en_US
dc.contributor.author Tkachenko, Nikolai V. en_US
dc.contributor.author Subbaiyan, Navaneetha K. en_US
dc.contributor.author Chitta, Raghu en_US
dc.contributor.author Zandler, Melvin E. en_US
dc.contributor.author Lemmetyinen, Helge en_US
dc.contributor.author D'Souza, Francis en_US
dc.date.accessioned 2012-02-06T17:15:44Z
dc.date.available 2012-02-06T17:15:44Z
dc.date.issued 2009-07-30 en_US
dc.identifier 19580310 en_US
dc.identifier 9890903 en_US
dc.identifier.citation The journal of physical chemistry. A. 2009 Jul 30; 113(30): 8478-89. en_US
dc.identifier.issn 1520-5215 en_US
dc.identifier.issn 1089-5639 en_US
dc.identifier.uri http://dx.doi.org/10.1021/jp9032194 en_US
dc.identifier.uri http://hdl.handle.net/10057/4255
dc.description Click on the DOI link below to access the article (may not be free). en_US
dc.description.abstract A self-assembled supramolecular triad, a model to mimic the photochemical events of photosynthetic antenna-reaction center, viz., sequential energy and electron transfer, has been newly constructed and studied. Boron dipyrrin, zinc porphyrin, and fullerene respectively constitute the energy donor, electron donor, and electron acceptor segments of the antenna-reaction center mimicry. For the construction, first, boron dipyrrin was covalently attached to a zinc porphyrin entity bearing a benzo-18-crown-6 host segment at the opposite end of the porphyrin ring. Next, an alkyl ammonium functionalized fullerene was used to self-assemble the crown ether entity via ion-dipole interactions. The newly formed supramolecular triad was fully characterized by spectroscopic, computational, and electrochemical methods. Selective excitation of the boron dipyrrin moiety in the dyad resulted in energy transfer over 97% efficiency creating singlet excited zinc porphyrin. The rate of energy transfer from the decay measurements of time-correlated singlet photon counting (TCSPC) and up-conversion techniques agreed well with that obtained by the pump-probe technique and revealed efficient photoinduced energy transfer in the dyad (time constant in the order of 10-60 ps depending upon the conformer). Upon forming the supramolecular triad by self-assembling fullerene, the excited zinc porphyrin resulted in electron transfer to the coordinated fullerene yielding a charge-separated state, thus mimicking the antenna-reaction center functionalities of photosynthesis. Nanosecond transient absorption studies yielded a lifetime of the charge-separated state to be 23 micros indicating charge stabilization in the supramolecular triad. The present supramolecular system represents a successful model to mimic the rather complex "combined antenna-reaction center" events of photosynthesis. en_US
dc.format.extent 8478-89 en_US
dc.language.iso eng en_US
dc.publisher American Chemical Society en_US
dc.relation.ispartofseries The journal of physical chemistry. A en_US
dc.relation.ispartofseries J Phys Chem A 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 Aminopyrine/chemistry en_US
dc.subject.mesh Biomimetic Materials/chemistry en_US
dc.subject.mesh Biomimetics en_US
dc.subject.mesh Boron/chemistry en_US
dc.subject.mesh Electron Transport en_US
dc.subject.mesh Energy Transfer en_US
dc.subject.mesh Fullerenes/chemistry en_US
dc.subject.mesh Macromolecular Substances/chemistry en_US
dc.subject.mesh Metalloporphyrins/chemistry en_US
dc.subject.mesh Molecular Mimicry en_US
dc.subject.mesh Photosynthetic Reaction Center Complex Proteins/chemistry en_US
dc.subject.mesh Zinc/chemistry en_US
dc.title Photosynthetic antenna-reaction center mimicry: sequential energy- and electron transfer in a self-assembled supramolecular triad composed of boron dipyrrin, zinc porphyrin and fullerene en_US
dc.type Article en_US
dc.coverage.spacial United States en_US
dc.description.version peer reviewed en_US
dc.rights.holder Copyright © 2009 American Chemical Society en_US

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