Electrically tuned hyperfine spectrum in neutral Tb(II)(Cp iPr5)2 single-molecule magnet
Abstract
Molecular spin qubits with long spin coherence time as well as non-invasive operation methods on such qubits are in high demand. It was shown that both molecular electronic and nuclear spin levels can be used as qubits. In solid state systems with dopants, an electric field was shown to effectively change the spacing between the nuclear spin qubit levels when the electron spin density is high at the nucleus of the dopant. Inspired by such solid-state systems, we propose that divalent lanthanide (Ln) complexes with an unusual electronic configuration of Ln2+ have a strong interaction between the Ln nuclear spin and the electronic degrees of freedom, which renders electrical tuning of the interaction. Furthermore, as an example, we study electronic structure and hyperfine interaction of the 159Tb nucleus in a neutral Tb(II)(CpiPr5)2 single-molecule magnet (SMM), which exhibits unusually long magnetization relaxation time, using the complete active space self-consistent field (CASSCF) method with spin–orbit interaction included within the restricted active space state interaction (RASSI). Our calculations show that the low-energy states arise from 4f8(6s,5dz2)1, 4f8(5dx2-y2)1, and 4f8(5dxy)1 configurations. We compute the hyperfine interaction parameters and the electronic–nuclear spectrum within our multiconfigurational approach. We find that the hyperfine interaction is about onemore »
- Authors:
-
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- Publication Date:
- Research Org.:
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); San Diego Supercomputer Center (SDSC)
- OSTI Identifier:
- 1852594
- Alternate Identifier(s):
- OSTI ID: 1664580
- Grant/Contract Number:
- SC0018326; DMR060009N
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 22; Journal Issue: 38; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Smith, Robert L., Wysocki, Aleksander L., and Park, Kyungwha. Electrically tuned hyperfine spectrum in neutral Tb(II)(Cp iPr5)2 single-molecule magnet. United States: N. p., 2020.
Web. doi:10.1039/d0cp04056h.
Smith, Robert L., Wysocki, Aleksander L., & Park, Kyungwha. Electrically tuned hyperfine spectrum in neutral Tb(II)(Cp iPr5)2 single-molecule magnet. United States. https://doi.org/10.1039/d0cp04056h
Smith, Robert L., Wysocki, Aleksander L., and Park, Kyungwha. Tue .
"Electrically tuned hyperfine spectrum in neutral Tb(II)(Cp iPr5)2 single-molecule magnet". United States. https://doi.org/10.1039/d0cp04056h. https://www.osti.gov/servlets/purl/1852594.
@article{osti_1852594,
title = {Electrically tuned hyperfine spectrum in neutral Tb(II)(Cp iPr5)2 single-molecule magnet},
author = {Smith, Robert L. and Wysocki, Aleksander L. and Park, Kyungwha},
abstractNote = {Molecular spin qubits with long spin coherence time as well as non-invasive operation methods on such qubits are in high demand. It was shown that both molecular electronic and nuclear spin levels can be used as qubits. In solid state systems with dopants, an electric field was shown to effectively change the spacing between the nuclear spin qubit levels when the electron spin density is high at the nucleus of the dopant. Inspired by such solid-state systems, we propose that divalent lanthanide (Ln) complexes with an unusual electronic configuration of Ln2+ have a strong interaction between the Ln nuclear spin and the electronic degrees of freedom, which renders electrical tuning of the interaction. Furthermore, as an example, we study electronic structure and hyperfine interaction of the 159Tb nucleus in a neutral Tb(II)(CpiPr5)2 single-molecule magnet (SMM), which exhibits unusually long magnetization relaxation time, using the complete active space self-consistent field (CASSCF) method with spin–orbit interaction included within the restricted active space state interaction (RASSI). Our calculations show that the low-energy states arise from 4f8(6s,5dz2)1, 4f8(5dx2-y2)1, and 4f8(5dxy)1 configurations. We compute the hyperfine interaction parameters and the electronic–nuclear spectrum within our multiconfigurational approach. We find that the hyperfine interaction is about one order of magnitude greater than that for Tb(III)Pc2 SMMs. This stems from the strong Fermi contact interaction between the Tb nuclear spin and the electron spin density at the nucleus that originates from the occupation of the (6s,5d) orbitals. We also uncover that the response of the Fermi contact term to electric field results in electrical tuning of the electronic–nuclear level separations. This hyperfine Stark effect may be useful for applications of molecular nuclear spins for quantum computing.},
doi = {10.1039/d0cp04056h},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 38,
volume = 22,
place = {United States},
year = {Tue Sep 15 00:00:00 EDT 2020},
month = {Tue Sep 15 00:00:00 EDT 2020}
}
Web of Science
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