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Entangled spin-polarized excitons from singlet fission in a rigid dimer

Author

Listed:
  • Ryan D. Dill

    (University of Colorado Boulder)

  • Kori E. Smyser

    (University of Colorado Boulder)

  • Brandon K. Rugg

    (National Renewable Energy Laboratory)

  • Niels H. Damrauer

    (University of Colorado Boulder
    University of Colorado Boulder)

  • Joel D. Eaves

    (University of Colorado Boulder
    University of Colorado Boulder)

Abstract

Singlet fission, a process that splits a singlet exciton into a biexciton, has promise in quantum information. We report time-resolved electron paramagnetic resonance measurements on a conformationally well-defined acene dimer molecule, TIPS-BP1', designed to exhibit strongly state-selective relaxation to specific magnetic spin sublevels. The resulting optically pumped spin polarization is a nearly pure initial state from the ensemble. The long-lived spin coherences modulate the signal intrinsically, allowing a measurement scheme that substantially removes noise and uncertainty in the magnetic resonance spectra. A nonadiabatic transition theory with a minimal number of spectroscopic parameters allows the quantitative assignment and interpretation of the spectra. In this work, we show that the rigid dimer TIPS-BP1' supports persistent spin coherences at temperatures far higher than those used in conventional superconducting quantum hardware.

Suggested Citation

  • Ryan D. Dill & Kori E. Smyser & Brandon K. Rugg & Niels H. Damrauer & Joel D. Eaves, 2023. "Entangled spin-polarized excitons from singlet fission in a rigid dimer," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36529-6
    DOI: 10.1038/s41467-023-36529-6
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    References listed on IDEAS

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    1. Daphné Lubert-Perquel & Enrico Salvadori & Matthew Dyson & Paul N. Stavrinou & Riccardo Montis & Hiroki Nagashima & Yasuhiro Kobori & Sandrine Heutz & Christopher W. M. Kay, 2018. "Identifying triplet pathways in dilute pentacene films," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
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