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Thousandfold Enhanc...
Thousandfold Enhancement of Photoreduction Lifetime in Re(bpy)(CO)(3) via Spin-Dependent Electron Transfer from a Perylenediimide Radical Anion Donor
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- Hedström, Svante (author)
- Stockholms universitet,Fysikum,Yale University, United States
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Chaudhuri, Subhajyoti (author)
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La Porte, Nathan T. (author)
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Rudshteyn, Benjamin (author)
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Martinez, Jose F. (author)
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Wasielewski, Michael R. (author)
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Batista, Victor S. (author)
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(creator_code:org_t)
- 2017-11-08
- 2017
- English.
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 139:46, s. 16466-16469
- Related links:
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https://www.osti.gov...
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Subject headings
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- 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.
Subject headings
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
- NATURVETENSKAP -- Fysik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences (hsv//eng)
Publication and Content Type
- ref (subject category)
- art (subject category)
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