Show simple item record

dc.contributorWichita State University. Department of Chemistryen_US
dc.contributor.authorMaligaspe, Erandaen_US
dc.contributor.authorTkachenko, Nikolai V.en_US
dc.contributor.authorSubbaiyan, Navaneetha K.en_US
dc.contributor.authorChitta, Raghuen_US
dc.contributor.authorZandler, Melvin E.en_US
dc.contributor.authorLemmetyinen, Helgeen_US
dc.contributor.authorD'Souza, Francisen_US
dc.identifier.citationThe journal of physical chemistry. A. 2009 Jul 30; 113(30): 8478-89.en_US
dc.descriptionClick on the DOI link below to access the article (may not be free).en_US
dc.description.abstractA 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.publisherAmerican Chemical Societyen_US
dc.relation.ispartofseriesThe journal of physical chemistry. Aen_US
dc.relation.ispartofseriesJ Phys Chem Aen_US
dc.subjectResearch Support, Non-U.S. Gov'ten_US
dc.subjectResearch Support, U.S. Gov't, Non-P.H.S.en_US
dc.subject.meshBiomimetic Materials/chemistryen_US
dc.subject.meshElectron Transporten_US
dc.subject.meshEnergy Transferen_US
dc.subject.meshMacromolecular Substances/chemistryen_US
dc.subject.meshMolecular Mimicryen_US
dc.subject.meshPhotosynthetic Reaction Center Complex Proteins/chemistryen_US
dc.titlePhotosynthetic antenna-reaction center mimicry: sequential energy- and electron transfer in a self-assembled supramolecular triad composed of boron dipyrrin, zinc porphyrin and fullereneen_US
dc.coverage.spacialUnited Statesen_US
dc.description.versionpeer revieweden_US
dc.rights.holderCopyright © 2009 American Chemical Societyen_US

Files in this item


There are no files associated with this item.

This item appears in the following Collection(s)

Show simple item record