Emergence of Interfacial Magnetism in Strongly‐Correlated Nickelate‐Titanate Superlattices

Abstract

Strongly‐correlated transition‐metal oxides are widely known for their various exotic phenomena. This is exemplified by rare‐earth nickelates such as LaNiO3, which possess intimate interconnections between their electronic, spin, and lattice degrees of freedom. Their properties can be further enhanced by pairing them in hybrid heterostructures, which can lead to hidden phases and emergent phenomena. An important example is the LaNiO3/LaTiO3 superlattice, where an interlayer electron transfer has been observed from LaTiO3 into LaNiO3 leading to a high‐spin state. However, macroscopic emergence of magnetic order associated with this high‐spin state has so far not been observed. Here, by using muon spin rotation, x‐ray absorption, and resonant inelastic x‐ray scattering, direct evidence of an emergent antiferromagnetic order with high magnon energy and exchange interactions at the LaNiO3/LaTiO3 interface is presented. As the magnetism is purely interfacial, a single LaNiO3/LaTiO3 interface can essentially behave as an atomically thin strongly‐correlated quasi‐2D antiferromagnet, potentially allowing its technological utilization in advanced spintronic devices. Furthermore, its strong quasi‐2D magnetic correlations, orbitally‐polarized planar ligand holes, and layered superlattice design make its electronic, magnetic, and lattice configurations resemble the precursor states of superconducting cuprates and nickelates, but with an S→1 spin state instead.