Spin-Electric Effect on a Chiral Dysprosium Complex

The Spin-Electric Effect (SEE) on molecules-the influence of external electric fields on molecular spin states-offers a compelling route toward low-power molecule-based spintronic applications. However, SEE remains elusive in molecular systems due to typically weak spin-electric field coupling. In this study, we observe a relevant SEE in a mononuclear lanthanide complex using Electric Field Modulated Electron Paramagnetic Resonance spectroscopy. We reveal a marked anisotropy of the SEE, evidencing that the most perturbed g tensor component is the one perpendicular to the electric field, providing hints for the most convenient experimental configuration to tune ad hoc spin transitions. Ab initio calculations in synergy with the experimental results revealed that molecular symmetry breaking plays a fundamental role. We also point out the crystal field parameters that are most strongly modulated by the presence of an electric field. These parameters are all off-diagonal, indicating effective electric-field-mediated state mixing.