9.2 GHz Clock Transition in a Lu(II) Molecular Spin Qubit Arising from a Massive 3467 MHz Hyperfine Interaction

ORAL

Abstract

Molecular spin qubits are attractive targets for next-generation quantum technologies [1] due to their intrinsic tunability via coordination chemistry techniques, enabling precise control of the relevant spin degrees of freedom and the possibility for massive scale-up via self-assembly. Here, we demonstrate chemical control of the degree of s-orbital mixing into the spin-bearing d-orbital associated with a series of spin-½ La(II) and Lu(II) molecules. Increased s-orbital character reduces spin-orbit coupling and enhances the electron-nuclear Fermi contact interaction. Both outcomes are beneficial for quantum applications: the former reduces spin-lattice relaxation, while the latter gives rise to a record molecular hyperfine interaction for Lu(II) that, in turn, generates a massive 9 GHz hyperfine clock transition and an order of magnitude increase in phase memory time [2]. These findings suggest new strategies for development of molecular quantum technologies, similar to trapped ion systems.

[1] Gaita-Ariño et al., Nat. Chem. 11, 301 – 309 (2019); https://doi.org/10.1038/s41557-019-0232-y

[2] Kundu et al., ChemRxiv 14399333 (Apr 2021). https://doi.org/10.26434/chemrxiv.14399333.v1

*We thank the U.S. National Science Foundation (under CHE-1855328 to WJE and CHE-1800431 to FF) and the Department of Energy (under DE-SC0020260 to SH) for support of this research. Work performed at the NHMFL is supported by the NSF (DMR-1644779) and by the State of Florida. JMY acknowledges support of the NSF Graduate Research Fellowship Program. We also thank the Eddleman Quantum Institute for promoting this collaborative project.

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Publication: Record 9.2 GHz hyperfine clock transition in a Lu(II) molecular spin qubit, Krishnendu Kundu, Jessica R. K. White, Samuel A. Moehring, Jason M. Yu, Joseph W. Ziller, Filipp Furche, William J. Evans, Stephen Hill, Nature Chemistry (under review).

Clock transition due to a record 1240 G hyperfine interaction in a Lu(II) molecular spin qubit, Krishnendu Kundu, Jessica R. K. White, Samuel A. Moehring, Jason M. Yu, Joseph W. Ziller, Filipp Furche, William J. Evans, and Stephen Hill, ChemRxiv 14399333 (Apr 2021). https://doi.org/10.26434/chemrxiv.14399333.v1

Presenters

  • Stephen Hill

    • Florida State University

Authors

  • Stephen Hill

    • Florida State University

  • Krishnendu Kundu

    • NHMFL, Florida State University

  • Jessica White

    • UC Irvine, Chemistry

  • Samuel Moehring

    • UC Irvine, Chemistry

  • Jason Yu

    • UC Irvine, Chemistry

  • Joseph Ziller

    • UC Irvine, Chemistry

  • Filipp Furche

    • UC Irvine, Chemistry

  • William Evans

    • UC Irvine, Chemistry
    • UC Irvine