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 Ln$^{2+}$ have a strong interaction between the Ln nuclear spin and the electronic degrees of freedom, which renders electrical tuning of the interaction. As an example, we study electronic structure and hyperfine interaction of the $^{159}$Tb nucleus in a neutral Tb(II)(Cp$^{\rm{iPr5}}$)$_2$ single-molecule magnet (SMM) using the complete active space self-consistent field method with spin-orbit interaction included within the restricted active space state interaction. Our calculations show that the low-energy states arise from $4f^8(6s,5d_{z^2})^1$, 4$f^8$(5$d_{x^2-y^2}$)$^1$, and $4f^8(5d_{xy})^1$ 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)Pc$_2$ 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.
Theory of Electrically Detected Magnetic Resonance of Silicon Vacancy-Related Spin Pairs in Silicon Carbide
University of Iowa（爱荷华大学）；Jet Propulsion Laboratory, California Institute of Technology（加州理工学院喷气推进实验室）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）；Coastal Carolina University（海岸卡罗来纳大学）；The Pennsylvania State University（宾夕法尼亚州立大学）；Eindhoven University of Technology（埃因霍温理工大学）
Separating hyperfine from spin-orbit interactions in organic semiconductors by multi-octave magnetic resonance using coplanar waveguide microresonators
Electrically detected magnetic resonance of $^{75}$As magnetic clock transitions in silicon
University of Melbourne（墨尔本大学）；University of Manchester（曼彻斯特大学）；University College London（伦敦大学学院）；RMIT University（皇家墨尔本理工大学）；Australian Research Council Centre for Quantum Computation and Communication Technology（澳大利亚研究委员会量子计算与通信技术中心）；CSIRO（联邦科学与工业研究组织）
Extraction of Isotropic Electron-Nuclear Hyperfine Coupling Constants of Paramagnetic Point Defects from Near-Zero Field Magnetoresistance Spectra via Least Squares Fitting to Models Developed from the Stochastic Quantum Liouville Equation
