Spin-Selective Photoreduction of a Stable Radical within a Covalent Donor-Acceptor-Radical Triad

Brandon K. Rugg, Brian T. Phelan, Noah E. Horwitz, Ryan M. Young, Matthew D. Krzyaniak, Mark A Ratner, Michael R Wasielewski

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

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+•-1(A-•-R), and subsequent reduction of R only occurs in D+•-1(A-•-R). These findings inform the design of multispin systems to transfer spin coherence between molecules targeting quantum information processing using the agency of SCRPs.

Original languageEnglish
Pages (from-to)15660-15663
Number of pages4
JournalJournal of the American Chemical Society
Volume139
Issue number44
DOIs
Publication statusPublished - Nov 8 2017

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Electrons
Automatic Data Processing
Perylene
Molecules
Photoexcitation
Chromophores
Anions
Negative ions
Statistics

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Spin-Selective Photoreduction of a Stable Radical within a Covalent Donor-Acceptor-Radical Triad. / Rugg, Brandon K.; Phelan, Brian T.; Horwitz, Noah E.; Young, Ryan M.; Krzyaniak, Matthew D.; Ratner, Mark A; Wasielewski, Michael R.

In: Journal of the American Chemical Society, Vol. 139, No. 44, 08.11.2017, p. 15660-15663.

Research output: Contribution to journalArticle

Rugg, Brandon K. ; Phelan, Brian T. ; Horwitz, Noah E. ; Young, Ryan M. ; Krzyaniak, Matthew D. ; Ratner, Mark A ; Wasielewski, Michael R. / Spin-Selective Photoreduction of a Stable Radical within a Covalent Donor-Acceptor-Radical Triad. In: Journal of the American Chemical Society. 2017 ; Vol. 139, No. 44. pp. 15660-15663.
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