Structure, Magnetism, and First-Principles Modeling of the Na0.5La0.5RuO3 Perovskite

High-purity polycrystalline Na0.5La0.5RuO3 was synthesized by a solid-state method, and its properties were studied by magnetic susceptibility, heat capacity, and resistivity measurements. We find it to be an orthorhombic perovskite, in contrast to an earlier report, with random La/Na mixing. With a Curie–Weiss temperature of −231 K and an effective moment of 2.74 μB/mol Ru, there is no magnetic ordering down to 1.8 K. A broad hump at 1.4 K in the heat capacity, however, indicates the presence of a glassy magnetic transition, which we attribute to the influence of the random distribution of Na and La on the perovskite A-sites. Comparison to CaRuO3, a structurally ordered ruthenate perovskite with a similar A-site ionic radius and magnetic properties, is presented. First-principles calculations indicate that the Na–La distribution determines the local magnetic exchange interactions between Ru ions, favoring either antiferromagnetic or ferromagnetic coupling when the local environment is Na- or La-rich. Thus, our data and analysis suggest that mixing cations with different charges and sizes on the A-site in this perovskite results in magnetic frustration through a balance of local magnetic exchange interactions.