Charges and spins in strongly correlated systems determine the electronic and magnetic structures, which define the cor responding electronic and magnetic pro perties. [1,2] Charge modulation, achieved through chemical and electrostatic doping, is a common technique to modify the band filling status. These modified elec tronic structures have an influence on the properties, e.g. high temperature super conductivity, electronic phase separation, and charge ordering. [2][3][4] Nonstoichiom etry, which commonly exists in materials, results in an unintentional doping, altering their properties. [5] For example, oxygen deficient SrTiO 3−x becomes conductive, [6] in contrary stoichiometric SrTiO 3 (STO) is a typical band insulator with a band gap of 3.2 eV. In manganite, [7,8] cobalt, [9,10] iron, and nickelbased perovskites, [11,12] the nonstoichiometry of oxygen not only introduces electron/hole doping but also affects the superexchange or double exchange interactions by modification of Interface-driven magnetic effects and phenomena associated with spin-orbit coupling and intrinsic symmetry breaking are of importance for fundamental physics and device applications. How interfaces affect the interplay between charge, spin, orbital, and lattice degrees of freedom is the key to boosting device performance. In LaMnO 3 /SrTiO 3 (LMO/STO) polar-nonpolar heterostructures, electronic reconstruction leads to an antiferromagnetic to ferromagnetic transition, making them viable for spin filter applications. The interfacial electronic structure plays a critical role in the understanding of the microscopic origins of the observed magnetic phase transition, from antiferromagnetic at 5 unit cells (ucs) of LMO or below to ferromagnetic at 6 ucs or above, yet such a study is missing. Here, an atomic scale understanding of LMO/STO ambipolar ferromagnetism is offered by quantifying the interface charge distribution and performing first-principles density functional theory (DFT) calculations across this abrupt magnetic transition. It is found that the electronic reconstruction is confined within the first 3 ucs of LMO from the interface, and more importantly, it is robust against oxygen nonstoichiometry. When restoring stoichiometry, an enhanced ferromagnetic insulating state in LMO films with a thickness as thin as 2 nm (5 uc) is achieved, making LMO readily applicable as barriers in spin filters.
Ambipolar FerromagnetismThe ORCID identification number(s) for the author(s) of this article can be found under https://doi.