Enhancing Spin Coherence of Optically-Addressed Molecular Qubit by Nuclear Spin Hyperpolarization

Fuente: arXiv
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Autores principales: Li, Boning, Hautle, Patrick, Zhang, Duhan, Zhu, Liangping, Beers, Ashley, Wang, Zeyu, Cappellaro, Paola, Wenckebach, Tom, Quan, Yifan
Formato: Preprint
Publicado: 2026
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author Li, Boning
Hautle, Patrick
Zhang, Duhan
Zhu, Liangping
Beers, Ashley
Wang, Zeyu
Cappellaro, Paola
Wenckebach, Tom
Quan, Yifan
author_facet Li, Boning
Hautle, Patrick
Zhang, Duhan
Zhu, Liangping
Beers, Ashley
Wang, Zeyu
Cappellaro, Paola
Wenckebach, Tom
Quan, Yifan
contents Optically addressable molecular triplet spins provide a chemically tunable platform for quantum application, but their coherence is often limited by interactions with surrounding spin baths. Here we demonstrate controlled suppression of nuclear-bath-induced decoherence in photoexcited triplet spins of pentacene co-crystallized in high-purity naphthalene single crystals. By hyperpolarizing the proton spin bath through triplet dynamic nuclear polarization (triplet-DNP), magnetic noise generated by the nuclear spins is suppressed, leading to an extension of the electron spin transverse coherence time. Experimentally, we observe a 25\% enhancement of the spin-echo decay time with $60\%$ polarization of the proton spin bath. The measured scaling of the spin-echo decay time ($T_2$) with nuclear polarization quantitatively follows the predicted dependence derived from the polarization-controlled nuclear second moment. Both the enhancement and the absolute value of the coherence time are quantitatively reproduced by cluster correlation expansion (CCE) simulations. These results establish nuclear spin hyperpolarization as a general and actively tunable approach to engineering coherence in molecular qubits. This work provides a broadly applicable design framework for high-coherence molecular and solid-state spin systems.
format Preprint
id arxiv_https___arxiv_org_abs_2603_27872
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Enhancing Spin Coherence of Optically-Addressed Molecular Qubit by Nuclear Spin Hyperpolarization
Li, Boning
Hautle, Patrick
Zhang, Duhan
Zhu, Liangping
Beers, Ashley
Wang, Zeyu
Cappellaro, Paola
Wenckebach, Tom
Quan, Yifan
Chemical Physics
Materials Science
Quantum Physics
Optically addressable molecular triplet spins provide a chemically tunable platform for quantum application, but their coherence is often limited by interactions with surrounding spin baths. Here we demonstrate controlled suppression of nuclear-bath-induced decoherence in photoexcited triplet spins of pentacene co-crystallized in high-purity naphthalene single crystals. By hyperpolarizing the proton spin bath through triplet dynamic nuclear polarization (triplet-DNP), magnetic noise generated by the nuclear spins is suppressed, leading to an extension of the electron spin transverse coherence time. Experimentally, we observe a 25\% enhancement of the spin-echo decay time with $60\%$ polarization of the proton spin bath. The measured scaling of the spin-echo decay time ($T_2$) with nuclear polarization quantitatively follows the predicted dependence derived from the polarization-controlled nuclear second moment. Both the enhancement and the absolute value of the coherence time are quantitatively reproduced by cluster correlation expansion (CCE) simulations. These results establish nuclear spin hyperpolarization as a general and actively tunable approach to engineering coherence in molecular qubits. This work provides a broadly applicable design framework for high-coherence molecular and solid-state spin systems.
title Enhancing Spin Coherence of Optically-Addressed Molecular Qubit by Nuclear Spin Hyperpolarization
topic Chemical Physics
Materials Science
Quantum Physics
url https://arxiv.org/abs/2603.27872