Strain-Tuned Magnetic Frustration in a Square Lattice $J_1$-$J_2$ Material

Commun. Phys. 7, 230 (2024) Magnetic frustration is a route that can lead to the emergence of novel ground states, including spin liquids and spin ices. Such frustration can be introduced through either the geometry of lattice structures or by incompatible exchange interactions. Identifying suitable strategies to control the degree of magnetic frustration in real systems is an active field of research. In this study, we devise a design principle for the tuning of frustrated magnetism on the square lattice through the manipulation of nearest (NN) and next-nearest neighbor (NNN) antiferromagnetic (AF) exchange interactions. By studying the magnon excitations in epitaxially-strained La$_2$NiO$_4$ films using resonant inelastic x-ray scattering (RIXS) we show that, in contrast to the cuprates, the dispersion peaks at the AF zone boundary. This indicates the presence of an AF-NNN spin interaction. Using first principles simulations and an effective spin-model, we demonstrate the AF-NNN coupling to be a consequence of the two-orbital nature of La$_2$NiO$_4$. Our results demonstrate that compressive strain can enhance this coupling, providing a design principle for the tunability of frustrated magnetism on a square lattice.