Your browser doesn't support javascript.
loading
Engineering Clock Transitions in Molecular Lanthanide Complexes.
Stewart, Robert; Canaj, Angelos B; Liu, Shuanglong; Regincós Martí, Emma; Celmina, Anna; Nichol, Gary; Cheng, Hai-Ping; Murrie, Mark; Hill, Stephen.
Afiliación
  • Stewart R; National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32310, United States.
  • Canaj AB; Department of Physics, Florida State University, Tallahassee, Florida 32306, United States.
  • Liu S; Center for Molecular Magnetic Quantum Materials, University of Florida, Gainesville, Florida 32611, United States.
  • Regincós Martí E; School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, U.K.
  • Celmina A; Center for Molecular Magnetic Quantum Materials, University of Florida, Gainesville, Florida 32611, United States.
  • Nichol G; Department of Physics, Northeastern University, Boston, Massachusetts 02115, United States.
  • Cheng HP; School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, U.K.
  • Murrie M; School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, U.K.
  • Hill S; EastCHEM School of Chemistry, The University of Edinburgh, David Brewster Road, Edinburgh EH9 3FJ, Scotland, U.K.
J Am Chem Soc ; 146(16): 11083-11094, 2024 Apr 24.
Article en En | MEDLINE | ID: mdl-38619978
ABSTRACT
Molecular lanthanide (Ln) complexes are promising candidates for the development of next-generation quantum technologies. High-symmetry structures incorporating integer spin Ln ions can give rise to well-isolated crystal field quasi-doublet ground states, i.e., quantum two-level systems that may serve as the basis for magnetic qubits. Recent work has shown that symmetry lowering of the coordination environment around the Ln ion can produce an avoided crossing or clock transition within the ground doublet, leading to significantly enhanced coherence. Here, we employ single-crystal high-frequency electron paramagnetic resonance spectroscopy and high-level ab initio calculations to carry out a detailed investigation of the nine-coordinate complexes, [HoIIIL1L2], where L1 = 1,4,7,10-tetrakis(2-pyridylmethyl)-1,4,7,10-tetraaza-cyclododecane and L2 = F- (1) or [MeCN]0 (2). The pseudo-4-fold symmetry imposed by the neutral organic ligand scaffold (L1) and the apical anionic fluoride ion generates a strong axial anisotropy with an mJ = ±8 ground-state quasi-doublet in 1, where mJ denotes the projection of the J = 8 spin-orbital moment onto the ∼C4 axis. Meanwhile, off-diagonal crystal field interactions give rise to a giant 116.4 ± 1.0 GHz clock transition within this doublet. We then demonstrate targeted crystal field engineering of the clock transition by replacing F- with neutral MeCN (2), resulting in an increase in the clock transition frequency by a factor of 2.2. The experimental results are in broad agreement with quantum chemical calculations. This tunability is highly desirable because decoherence caused by second-order sensitivity to magnetic noise scales inversely with the clock transition frequency.
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos