Molecular Cocrystal Packing Suppresses Hopping-Driven Decoherence of Excitonic Spin Qubits DOI
Jonathan R. Palmer, Samuel B. Tyndall, Georgia Mantel

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: May 7, 2025

Molecular excitonic spins have garnered significant interest for quantum technologies because they can be initialized into addressable, multilevel states through spin-selective intersystem crossing or singlet fission. However, spin coherence is difficult to maintain above liquid helium temperatures due typical crystal packings, which promote decoherence exciton hopping between magnetically inequivalent sites. Here, we engineer donor-acceptor cocrystals where molecular packing in isolated π-stacks of equivalent molecules suppresses hopping-induced decoherence. Pulse-electron paramagnetic resonance spectroscopy reveals that high-temperature this geometry instead strongly influenced by mutual flip-flops interacting excitons. Coherence anisotropy measurements indicate spin-phonon coupling enhances the rate dynamic reorientation zero field splitting tensor. As a result, times decrease exponentially at elevated temperatures, with measurable up 150 K. The combined results present generalized design strategies preserve high temperatures.

Language: Английский

Molecular Cocrystal Packing Suppresses Hopping-Driven Decoherence of Excitonic Spin Qubits DOI
Jonathan R. Palmer, Samuel B. Tyndall, Georgia Mantel

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: May 7, 2025

Molecular excitonic spins have garnered significant interest for quantum technologies because they can be initialized into addressable, multilevel states through spin-selective intersystem crossing or singlet fission. However, spin coherence is difficult to maintain above liquid helium temperatures due typical crystal packings, which promote decoherence exciton hopping between magnetically inequivalent sites. Here, we engineer donor-acceptor cocrystals where molecular packing in isolated π-stacks of equivalent molecules suppresses hopping-induced decoherence. Pulse-electron paramagnetic resonance spectroscopy reveals that high-temperature this geometry instead strongly influenced by mutual flip-flops interacting excitons. Coherence anisotropy measurements indicate spin-phonon coupling enhances the rate dynamic reorientation zero field splitting tensor. As a result, times decrease exponentially at elevated temperatures, with measurable up 150 K. The combined results present generalized design strategies preserve high temperatures.

Language: Английский

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