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

Nguyen, Loi T.; Saubanère, Matthieu; Zhang, Qiang; Cava, Robert J.

doi:10.1021/acs.chemmater.0c03775

Title: Structure, Magnetism, and First-Principles Modeling of the Na_0.5La_0.5RuO₃ Perovskite

Journal Article · 13 January 2021 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.0c03775 · OSTI ID:1767850

^[1];

^[2];

^[3]; Cava, Robert J. ^[1]

Princeton Univ., NJ (United States)
Univ. de Montpellier (France)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division

High-purity polycrystalline Na_0.5La_0.5RuO₃ was synthesized by a solid-state method, and its properties were studied by magnetic susceptibility, heat capacity, and resistivity measurements. In this study, 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; FG02-98ER45706

OSTI ID:: 1767850

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 2 Vol. 33; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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Title: Structure, Magnetism, and First-Principles Modeling of the Na_0.5La_0.5RuO₃ Perovskite