The proximity effect is used to engineer interface effects such as magnetoelectric coupling, exchange bias, and emergent interfacial magnetism. However, the presence of a magnetic “dead layer” adversely affects the functionality of a heterostructure. Here, it is shown that by utilizing (111) polar planes, the magnetization of a manganite ultrathin layer can be maintained throughout its thickness. Combining structural characterization, magnetometry measurements, and magnetization depth profiling with polarized neutron reflectometry, it is found that the magnetic dead layer is absent in the (111)‐oriented manganite layers, however, it occurs in the films with other orientations. Quantitative analysis of local structural and elemental spatial evolutions using scanning transmission electron microscopy and electron energy loss spectroscopy reveals that atomically sharp interfaces with minimal chemical intermixing in the (111)‐oriented superlattices. The polar discontinuity across the (111) interfaces inducing charge redistribution within the SrTiO3 layers is suggested, which promotes ferromagnetism throughout the (111)‐oriented ultrathin manganite layers. The approach of eliminating problematic magnetic dead layers by changing the crystallographic orientation suggests a conceptually useful recipe to engineer the intriguing physical properties of oxide interfaces, especially in low dimensionality.

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intriguing physical magnetic dead layers polar discontinuity crystallographic orientation ferromagnetism polarized neutron reflectometry magnetization depth profiling electron energy loss spectroscopy manganite ultrathin layer emergent interfacial magnetism chemical intermixing proximity effect structural characterization magnetometry measurements scanning transmission electron microscopy dimensionality oxide interfaces magnetoelectric coupling exchange bias charge redistribution heterostructure local structural and elemental spatial evolutions interface effects

Er‐Jia Guo , Manuel A. Roldan , Timothy Charlton , Zhaoliang Liao , Qiang Zheng , Haile Ambaye , Andreas Herklotz , Zheng Gai , T. Zac Ward , Ho Nyung Lee , Michael R. Fitzsimmons,.Removal of the Magnetic Dead Layer by Geometric Design. 28 (28),.

Er‐Jia Guo , Manuel A. Roldan , Timothy Charlton , Zhaoliang Liao , Qiang Zheng , Haile Ambaye , Andreas Herklotz , Zheng Gai , T. Zac Ward , Ho Nyung Lee , Michael R. Fitzsimmons,"Removal of the Magnetic Dead Layer by Geometric Design" 28

Er‐Jia Guo , Manuel A. Roldan , Timothy Charlton , Zhaoliang Liao , Qiang Zheng , Haile Ambaye , Andreas Herklotz , Zheng Gai , T. Zac Ward , Ho Nyung Lee , Michael R. Fitzsimmons,"Removal of the Magnetic Dead Layer by Geometric Design"