Mean field magnetism and spin frustration in a double perovskite oxide with compositional complexity

Abstract

The rise of high-entropy oxides as a major functional materials design principle in recent years has prompted us to investigate how compositional disorder affects long-range magnetic ordering in double perovskite oxides. Since ferromagnetic insulators are emerging as an important platform for lossless spintronics, we consider the $RE_2$NiMnO$_6$ ($RE$ : rare-earth) family and investigate single-crystalline films of (La$_{0.4}$Nd$_{0.4}$Sm$_{0.4}$Gd$_{0.4}$Y$_{0.4}$)NiMnO$_{6}$ grown on SrTiO$_3$ (001) substrates in this work. Despite configurational disorder and high cationic size variance at the $RE$ site, the material exhibits robust ferromagnetic ordering with a Curie temperature ($T_\mathrm{c}$) of approximately 150 K. This $T_\mathrm{c}$ is consistent with the expectation based on consideration of the average ionic radii of the rare-earth ($RE$) sites in the bulk $RE_2$NiMnO$_6$. Below $T_\mathrm{c}$, Raman spectroscopy measurement finds a deviation from anharmonic behavior, where the phonon renormalization aligns with a mean-field approximation of spin-spin correlation. At lower temperature, magnetic $RE$ ions also contributed to the magnetic behavior and the system displays a reentrant spin-glass-like behavior. This study demonstrates that while a mean-field approach serves as a viable starting point for predicting the long-range transition temperature, microscopic details of the complex magnetic interactions are essential for understanding the low-temperature phase.