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*

*Corresponding author for this work

Research output: Contribution to journalArticle

14 Scopus citations

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 (US)
Pages (from-to)15660-15663
Number of pages4
JournalJournal of the American Chemical Society
Volume139
Issue number44
DOIs
StatePublished - Nov 8 2017

ASJC Scopus subject areas

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

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