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210411 LuCT ChemRxiv Final.pdf (3.93 MB)

Clock Transition Due to a Record 1240 G Hyperfine Interaction in a Lu(II) Molecular Spin Qubit

preprint
submitted on 12.04.2021, 01:49 and posted on 12.04.2021, 13:29 by Krishnendu Kundu, Jessica R. K. White, Samuel A. Moehring, Jason M. Yu, Joseph W. Ziller, Filipp Furche, William J. Evans, Stephen Hill
Spins in molecules are particularly attractive targets for next-generation quantum technologies, enabling chemically programmable qubits and potential for 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. These findings suggest new strategies for development of molecular quantum technologies, akin to trapped ion systems.

Funding

NSF CHE-1855328

NSF CHE-1800431

DOE DE-SC0020260

NSF DMR-1644779

History

Email Address of Submitting Author

shill@magnet.fsu.edu

Institution

Florida State University and NHMFL

Country

USA

ORCID For Submitting Author

0000-0001-6742-3620

Declaration of Conflict of Interest

No conflict of interest.

Version Notes

This is the first version of the pre-print

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