Full metadata record
DC Field | Value | Language |
---|---|---|
dc.contributor.author | Shunichi Fukuzumi | * |
dc.date.accessioned | 2016-08-28T12:08:34Z | - |
dc.date.available | 2016-08-28T12:08:34Z | - |
dc.date.issued | 2012 | * |
dc.identifier.issn | 2041-6520 | * |
dc.identifier.other | OAK-8200 | * |
dc.identifier.uri | https://dspace.ewha.ac.kr/handle/2015.oak/222133 | - |
dc.description.abstract | The exceptionally long lived charge separation previously observed in a β,β′-pyrrolic-fused ferrocene-porphyrin-fullerene triad (lifetime 630 μs) and related porphyrin-fullerene dyad (lifetime 260 μs) is attributed to the production of triplet charge-separated states. Such molecular excited-state spin polarization maintained over distances of up to 23 Å is unprecedented and offers many technological applications. Electronic absorption and emission spectra, femtosecond and nanosecond time-resolved transient absorption spectra, and cyclic voltammograms of two triads and four dyads are measured and analyzed to yield rate constants, donor-acceptor couplings, free-energy changes, and reorganization energies for charge-separation and charge-recombination processes. Production of long-lived intramolecular triplet states is confirmed by electron-paramagnetic resonance spectra at 77-223 K, as is retention of spin polarization in π-conjugated ferrocenium ions. The observed rate constants were either first predicted (singlet manifold) or later confirmed (triplet manifold) by a priori semiclassical kinetics calculations for all conceivable photochemical processes, parameterized using density-functional theory and complete-active-space self-consistent-field calculations. Identified are both a ps-timescale process attributed to singlet recombination and a μs-timescale process attributed to triplet recombination. © 2012 The Royal Society of Chemistry. | * |
dc.language | English | * |
dc.title | Long-lived long-distance photochemically induced spin-polarized charge separation in β,β′-pyrrolic fused ferrocene-porphyrin-fullerene systems | * |
dc.type | Article | * |
dc.relation.issue | 1 | * |
dc.relation.volume | 3 | * |
dc.relation.index | SCI | * |
dc.relation.index | SCIE | * |
dc.relation.index | SCOPUS | * |
dc.relation.startpage | 257 | * |
dc.relation.lastpage | 269 | * |
dc.relation.journaltitle | Chemical Science | * |
dc.identifier.doi | 10.1039/c1sc00614b | * |
dc.identifier.wosid | WOS:000297473200034 | * |
dc.identifier.scopusid | 2-s2.0-82455219506 | * |
dc.author.google | Lee S.-H. | * |
dc.author.google | Larsen A.G. | * |
dc.author.google | Ohkubo K. | * |
dc.author.google | Cai Z.-L. | * |
dc.author.google | Reimers J.R. | * |
dc.author.google | Fukuzumi S. | * |
dc.author.google | Crossley M.J. | * |
dc.contributor.scopusid | Shunichi Fukuzumi(35430038100;58409757400) | * |
dc.date.modifydate | 20240401081001 | * |