Abstract

AbstractGraphene, with spin and valley degrees of freedom, fosters unexpected physical and chemical properties for the realization of next‐generation quantum devices. However, the spin‐symmetry of graphene is rather robustly protected, hampering manipulation of the spin degrees of freedom for the application of spintronic devices such as electric gate‐tunable spin filters. It is demonstrated that a hybrid heterostructure composed of graphene and LaCoO3 epitaxial thin film exhibits an electrically tunable spin‐exchange splitting. The large and adjustable spin‐exchange splitting of 155.9 – 306.5 meV is obtained by the characteristic shifts in both the spin‐symmetry‐broken quantum Hall states and the Shubnikov–de Haas oscillations. Strong hybridization‐induced charge transfer across the hybrid heterointerface has been identified for the observed spin exchange splitting. The substantial and facile controllability of the spin exchange splitting provides an opportunity for spintronics applications with the electrically‐tunable spin polarization in hybrid heterostructures.

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