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Thousandfold Enhancement of Photoreduction Lifetime in Re(bpy)(CO)(3) via Spin-Dependent Electron Transfer from a Perylenediimide Radical Anion Donor
Stockholm University, Faculty of Science, Department of Physics. Yale University, United States.ORCID iD: 0000-0001-6496-6865
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Number of Authors: 7
2017 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 139, no 46, 16466-16469 p.Article in journal (Refereed) Published
Abstract [en]

Spin-dependent intramolecular electron transfer is revealed in the Re-I(CO)(3)(py)(bpy-Ph)perylenediimide radical anion (Re-I-bpy-PDI-(.)) dyad, a prototype model system for artificial photosynthesis. Quantum chemical calculations and ultrafast transient absorption spectroscopy experiments demonstrate that selective photoexcitation of Re-I-bpy results in electron transfer from PD-(.) to Re-I-bpy, forming two distinct charge-shifted states. One is an overall doublet whose return to the ground state is spin-allowed. The other, high spin quartet state, persists for 67 ns due to spin-forbidden back-electron transfer, constituting a more than thousandfold lifetime improvement compared to the low-spin state. Exploiting this spin dependency holds promise for artificial photosynthetic systems requiring long-lived reduced states to perform multi-electron chemistry.

Place, publisher, year, edition, pages
2017. Vol. 139, no 46, 16466-16469 p.
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Chemical Sciences Physical Sciences
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URN: urn:nbn:se:su:diva-150899DOI: 10.1021/jacs.7b09438ISI: 000416496400010PubMedID: 29083146OAI: oai:DiVA.org:su-150899DiVA: diva2:1171623
Available from: 2018-01-08 Created: 2018-01-08 Last updated: 2018-01-08Bibliographically approved

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