Oriented Triplet Excitons as Long-Lived Electron Spin Qutrits in a Molecular Donor-Acceptor Single Cocrystal

Jonathan R. Palmer, Malik L. Williams, Ryan M. Young, Kathryn R. Peinkofer, Brian T. Phelan, Matthew D. Krzyaniak*, Michael R. Wasielewski*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

3 Scopus citations


The photogeneration of multiple unpaired electron spins within molecules is a promising route to applications in quantum information science because they can be initialized into well-defined, multilevel quantum states (S > 1/2) and reproducibly fabricated by chemical synthesis. However, coherent manipulation of these spin states is difficult to realize in typical molecular systems due to the lack of selective addressability and short coherence times of the spin transitions. Here, these challenges are addressed by using donor-acceptor single cocrystals composed of pyrene and naphthalene dianhydride to host spatially oriented triplet excitons, which exhibit promising photogenerated qutrit properties. Time-resolved electron paramagnetic resonance (TREPR) spectroscopy demonstrates that spatially orienting triplet excitons in a single crystal platform imparts narrow, well-resolved, tunable resonances in the triplet EPR spectrum, allowing selective addressability of the spin sublevel transitions. Pulse-EPR spectroscopy reveals that at temperatures above 30 K, spin decoherence of these triplet excitons is driven by exciton diffusion. However, coherence is limited by electronic spin dipolar coupling below 30 K, where T2 varies nonlinearly with the optical excitation density due to exciton annihilation. Overall, an optimized coherence time of T2 = 7.1 μs at 20 K is achieved. These results provide important insights into designing solid-state molecular excitonic materials with improved spin qutrit properties.

Original languageEnglish (US)
Pages (from-to)1089-1099
Number of pages11
JournalJournal of the American Chemical Society
Issue number1
StatePublished - Jan 10 2024

ASJC Scopus subject areas

  • General Chemistry
  • Biochemistry
  • Catalysis
  • Colloid and Surface Chemistry


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