Spin-Selective Photoreduction of a Stable Radical within a Covalent Donor–Acceptor–Radical Triad
| Autor: | Brandon K. Rugg, Matthew D. Krzyaniak, Mark A. Ratner, Noah E. Horwitz, Michael R. Wasielewski, Ryan M. Young, Brian T. Phelan |
|---|---|
| Rok vydání: | 2017 |
| Předmět: |
Chemistry
Electron donor 02 engineering and technology General Chemistry Chromophore 010402 general chemistry 021001 nanoscience & nanotechnology Photochemistry 01 natural sciences Biochemistry Acceptor Catalysis 0104 chemical sciences chemistry.chemical_compound Electron transfer Colloid and Surface Chemistry Covalent bond Molecule Condensed Matter::Strongly Correlated Electrons Singlet state Physics::Chemical Physics 0210 nano-technology Perylene |
| Zdroj: | Journal of the American Chemical Society. 139:15660-15663 |
| ISSN: | 1520-5126 0002-7863 |
| Popis: | Controlling spin–spin interactions in multispin molecular assemblies is important for developing new approaches to quantum information processing. In this work, a covalent electron donor–acceptor–radical triad is used to probe spin-selective reduction of the stable radical to its diamagnetic anion. The molecule consists of a perylene electron donor chromophore (D) bound to a pyromellitimide acceptor (A), which is, in turn, linked to a stable α,γ-bisdiphenylene-β-phenylallyl radical (R•) to produce D-A-R•. Selective photoexcitation of D within D-A-R• results in ultrafast electron transfer to form the D+•-A–•-R• triradical, where D+•-A–• is a singlet spin-correlated radical pair (SCRP), in which both SCRP spins are uncorrelated relative to the R• spin. Subsequent ultrafast electron transfer within the triradical forms D+•-A-R–, but its yield is controlled by spin statistics of the uncorrelated A–•-R• radical pair, where the initial charge separation yields a 3:1 statistical mixture of D+•-3(A–•-R•) and D+•-... |
| Databáze: | OpenAIRE |
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