Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms

Karimi, Homa; Wysocki, Aleksander L.; Park, Kyungwha

doi:10.1021/acsnano.4c16416

Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms

Journal Article · Mon Apr 21 00:00:00 EDT 2025 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.4c16416· OSTI ID:2564470

Karimi, Homa ^[1]; ^[2]; ^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
University of Nebraska at Kearney, NE (United States)

Rare-earth adatoms on surfaces have been studied for potential atomic-scale magnetic storage, quantum sensing, and quantum computing applications. Despite accumulating experimental efforts, a comprehensive description of the electronic configurations of the adatoms remains elusive. Here, we investigate two charge states and several electronic configurations, including 5d and 6s valence shells, for a Sm adatom on a MgO substrate using multiconfigurational ab initio methods, for the possibility of using the Sm nuclear spin levels as qubits. For the configurations in a neutral charge state, we find that the electronic ground state is a singlet, and thus the hyperfine interaction associated with the ¹⁴⁷Sm nucleus is absent, which may greatly enhance nuclear spin coherence time. The degeneracy of the nuclear levels is lifted by the nuclear quadrupole interaction. We show that the splitting of the nuclear levels can be controlled by a static electric field, and that Rabi oscillations between the nuclear levels can be induced by a time-dependent electric field. For the configurations in a singly charged state, electronic Kramers doublets are formed. The electronic configurations including an unpaired 6s orbital exhibit a strong hyperfine Stark effect due to a large Fermi contact contribution to the hyperfine interaction. In these configurations, electric-field-induced Rabi oscillations between the electronic-nuclear levels can occur at frequencies up to 3 orders of magnitude higher than those for the neutral charge state. The proposed system may be experimentally observed within scanning tunneling microscopy.

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Research Organization:: Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0018326

OSTI ID:: 2564470

Alternate ID(s):: OSTI ID: 2564683

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 17 Vol. 19; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
electric fields
electrical control
hyperfine coupling
magnetic properties
multiconfigurational ab initio
nuclear spin qubits
oscillation
quantum mechanics
rare-earth adatoms

Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms

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