Rare-earth oxysulfides RE$_2$O$_2$S as model mixed-anion frustrated magnets

Abstract

The study of low-dimensional and anisotropic magnetism is a promising avenue for the discovery of novel quantum phenomena. Mixed-anion materials, defined by the coordination of metal cations by two or more distinct anionic species, provide an intrinsically anisotropic platform for the tuning of structural, magnetic, and electronic properties. In this work, we report the synthesis and characterization of a family of rare-earth oxysulfide (RE$_2$O$_2$S) antiferromagnets (AFM) possessing a triangular-bilayer slab lattice geometry. Long-range AFM order is observed for the majority of compositions, with several (RE = Ce, Pr, Nd, Sm) having been previously unreported. Although assumed to form stoichiometrically, pair distribution function (PDF) analysis provides evidence for significant, synthesis-dependent interslab structural disorder as RE$_2$O$_{2+x}$S$_{1-x}$, resulting in significant variability in the bulk magnetic response of the Nd member. This work highlights the tunability of frustrated magnetic ground states in rare-earth-based mixed-anion materials, and the importance of thorough structural characterization in the discovery of new mixed-anion magnets.