Ferromagnetic Insulating Ground-State Resolved in Mixed Protons and Oxygen Vacancies-Doped La_0.67Sr_0.33CoO₃ Thin...

The realization of ferromagnetic insulating ground state is a critical prerequisite for spintronic applications. By applying electric field-controlled ionic liquid gating (ILG) to stoichiometry La_0.67Sr_0.33CoO₃ thin films, the doping of protons (H⁺) has been achieved for the first time. Furthermore, a hitherto-unreported ferromagnetic insulating phase with a remarkably high T_c up to 180 K has been observed which can be attributed to the doping of H⁺ and the formation of oxygen vacancies (V_O). The chemical formula of the dual-ion migrated film has been identified as La_2/3Sr_1/3CoO_8/3H_2/3 based on combined Co L₂₃-edge absorption spectra and configuration interaction cluster calculations, from which we are able to explain the ferromagnetic ground state in terms of the distinct magnetic moment contributions from Co ions with octahedral (O_h) and tetrahedral (T_d) symmetries following antiparallel spin alignments. Further density functional theory calculations have been performed to verify the functionality of H⁺ as the transfer ion and the origin of the novel ferromagnetic insulating ground state. Our results provide a fundamental understanding of the ILG regulation mechanism and shed light on the manipulating of more functionalities in other correlated compounds through dual-ion manipulation.