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

Ryan D. Dill, Kori E. Smyser, Brandon K. Rugg, Niels H. Damrauer () and Joel D. Eaves ()
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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
Joel D. Eaves: University of Colorado Boulder

Nature Communications, 2023, vol. 14, issue 1, 1-7

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-36529-6

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