The frustrated FCC antiferromagnet Ba2YOsO6: structural characterization, magnetic properties and neutron scattering studies

preprint2014arXivOpen access

Abstract

We report the crystal structure, magnetization and neutron scattering measurements on the double perovskite Ba2_2YOsO6_6. The Fm3‾mFm\overline{3}m space group is found both at 290~K and 3.5~K with cell constants a0=8.3541(4)a_0 = 8.3541(4)~Å and 8.3435(4)8.3435(4)~Å, respectively. Os5+^{5+} (5d35d^3) ions occupy a non-distorted, geometrically frustrated face-centered-cubic (FCC) lattice. A Curie-Weiss temperature θ=−772θ= -772~K suggests the presence of a large antiferromagnetic interaction and a high degree of magnetic frustration. A magnetic transition to long range antiferromagnetic order, consistent with a Type I FCC state below TN∼69T_{\rm N} \sim 69~K, is revealed by magnetization, Fisher heat capacity and elastic neutron scattering, with an ordered moment of 1.65(6)~μBμ_B on Os5+^{5+}. The ordered moment is much reduced from either the expected spin only value of ∼3μB\sim 3 μ_B or the value appropriate to 4d34d^3 Ru5+^{5+} in isostructural Ba2_2YRuO6_6 of 2.2(1)~μBμ_B, suggesting a role for spin orbit coupling (SOC). Triple axis neutron scattering measurements of the order parameter suggest an additional first-order transition at T=67.45T = 67.45~K, and the existence of a second ordered state. % Time-of-flight inelastic neutron results reveal a large spin gap Δ∼17Δ\sim 17~meV, unexpected for an orbitally quenched, d3d^3 electronic configuration. We discuss this in the context of the ∼5\sim 5~meV spin gap observed in the related Ru5+^{5+}, 4d34d^3 cubic double perovskite Ba2_2YRuO6_6, and attribute the ∼3\sim 3 times larger gap to stronger SOC present in this heavier, 5d5d, osmate system.

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