Spin-Electric Coupling with Anisotropy-Induced Vanishment andEnhancement in Molecular Ferroelectrics

Manipulating quantum properties by electric fields using spin-electric coupling (SEC) effects promises spatialaddressability. While several studies about inorganic materialsshowing the SEC functionality have been reported, the vastlytunable crystal structures of molecular ferroelectrics provide arange of rationally designable materials yet to be exploited. In thiswork, Mn2+-doped molecular ferroelectrics are chosen toexperimentally demonstrate the feasibility of achieving thequantum coherent SEC effect in molecular ferroelectrics for thefirst time. The electricfield pulse applied between Hahn-echopulses in electron paramagnetic resonance (EPR) experimentscauses controllable phase shifts via manipulating of the zero-fieldsplitting (ZFS) of the Mn(II) ions. Detailed investigations of theaMn crystal showed unexpected SEC vanishment and enhancement at different crystal orientations, which were elucidated bystudying the spin Hamiltonian and magnetic anisotropy. With the enhanced SEC efficiency being achieved (0.68 Hz m/V), this workdiscovers an emerging material library of molecular ferroelectrics to implement coherent quantum control with selective and tunableSEC effects toward highly scalable quantum gates