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Manipulating magnetic anisotropy in complex oxide heterostructures has attracted much attention. Here, three interface‐engineering approaches are applied to address two general issues with controlling magnetic anisotropy in the La2/3Sr1/3MnO3 heterostructure. One is the paradox arising from the competition between Mn3d–O2p orbital hybridization and MnO6 crystal field. The other is the interfacial...
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