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Molecular spin qubits with long spin coherence time as well as non-invasiveoperation methods on such qubits are in high demand. It was shown that bothmolecular electronic and nuclear spin levels can be used as qubits. In solidstate systems with dopants, an electric field was shown to effectively changethe spacing between the nuclear spin qubit levels when the electron spindensity is high at the nucleus of the dopant. Inspired by such solid-statesystems, we propose that divalent lanthanide (Ln) complexes with an unusualelectronic configuration of Ln$^{2+}$ have a strong interaction between the Lnnuclear spin and the electronic degrees of freedom, which renders electricaltuning of the interaction. As an example, we study electronic structure andhyperfine interaction of the $^{159}$Tb nucleus in a neutralTb(II)(Cp$^{\rm{iPr5}}$)$_2$ single-molecule magnet (SMM) using the completeactive space self-consistent field method with spin-orbit interaction includedwithin the restricted active space state interaction. Our calculations showthat 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 computethe hyperfine interaction parameters and the electronic-nuclear spectrum withinour multiconfigurational approach. We find that the hyperfine interaction isabout one order of magnitude greater than that for Tb(III)Pc$_2$ SMMs. Thisstems from the strong Fermi contact interaction between the Tb nuclear spin andthe electron spin density at the nucleus that originates from the occupation ofthe $(6s,5d)$ orbitals. We also uncover that the response of the Fermi contactterm to electric field results in electrical tuning of the electronic-nuclearlevel separations. This hyperfine Stark effect may be useful for applicationsof molecular nuclear spins for quantum computing.

Electrically tuned hyperfine spectrum in neutral Tb(II)(Cp$^{\rm{iPr5}}$)$_2$ single-molecule magnet