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DOE OSTI · 1959403

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

Dill, Ryan D. (ORCID:0000000209546574)·Smyser, Kori E. (ORCID:0000000236970717)·Rugg, Brandon K.·Damrauer, Niels H. (ORCID:0000000183379375)·Eaves, Joel D. (ORCID:0000000293711703)
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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.

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72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDSelectron paramagnetic resonancemolecular photophysicsquantum information sciencesinglet fission

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BibTeXRIS

Dill, Ryan D. (ORCID:0000000209546574), Smyser, Kori E. (ORCID:0000000236970717), Rugg, Brandon K., Damrauer, Niels H. (ORCID:0000000183379375), Eaves, Joel D. (ORCID:0000000293711703). 2023-03-02. Entangled spin-polarized excitons from singlet fission in a rigid dimer. https://doi.org/10.1038/s41467-023-36529-6

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