Emergence of interfacial magnetism in strongly-correlated nickelate-titanate superlattices

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 and is predicted to result in a high-spin state. However, macroscopic emergence of magnetic order has so far not been observed. Here, by using muon spin rotation, x-ray absorption, and resonant inelastic x-ray scattering, we present direct evidence of an emergent antiferromagnetic order with high magnon energy and exchange interactions at the LaNiO₃/LaTiO₃ interface. As the magnetism is purely interfacial, a single LaNiO₃/LaTiO₃ interface can essentially behave as an atomically thin quasi-two-dimensional antiferromagnet, potentially allowing its technological utilisation in advanced spintronic devices. Furthermore, its strong quasi-two-dimensional magnetic correlations and orbitally-polarized planar ligand holes make its electronic and magnetic configurations resemble the precursor states of superconducting cuprates and nickelates, but with an S → 1 spin state instead.