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

Abstract

We report the crystal structure, magnetization and neutron scattering measurements on the double perovskite Ba${}_2$YOsO${}_6$. The $Fm\overline{3}m$ space group is found both at 290~K and 3.5~K with cell constants $a_0=8.3541(4)$~Å and $8.3435(4)$~Å, respectively. Os${}^{5+}$ ($5d^3$) ions occupy a non-distorted, geometrically frustrated face-centered-cubic (FCC) lattice. A Curie-Weiss temperature $\theta =-772$~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 $T_{\mathrm{N}}\sim 69$~K, is revealed by magnetization, Fisher heat capacity and elastic neutron scattering, with an ordered moment of 1.65(6)~${\mu }_B$ on Os${}^{5+}$. The ordered moment is much reduced from either the expected spin only value of $\sim 3{\mu }_B$ or the value appropriate to $4d^3$ Ru${}^{5+}$ in isostructural Ba${}_2$YRuO${}_6$ of 2.2(1)~${\mu }_B$, suggesting a role for spin orbit coupling (SOC). Triple axis neutron scattering measurements of the order parameter suggest an additional first-order transition at $T=67.45$~K, and the existence of a second ordered state. % Time-of-flight inelastic neutron results reveal a large spin gap $\Delta \sim 17$~meV, unexpected for an orbitally quenched, $d^3$ electronic configuration. We discuss this in the context of the $\sim 5$~meV spin gap observed in the related Ru${}^{5+}$, $4d^3$ cubic double perovskite Ba${}_2$YRuO${}_6$, and attribute the $\sim 3$ times larger gap to stronger SOC present in this heavier, $5d$, osmate system.

arXiv comment10 pages, 9 figures

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• Coulomb Correlations in 4d and 5d Oxides from First Principles - or How Spin-Orbit Materials choose their Effective Orbital Degeneracies
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• Octupolar order in d-orbital Mott insulators
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• Spin-orbit coupling controlled $J=3/2$ electronic ground state in 5$d^3$ oxides
• Multipolar magnetism in d-orbital systems: Crystal field levels, octupolar order, and orbital loop currents
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• Highly-anisotropic exchange interactions of $j_{\mathrm{eff}}=1/2$ iridium moments on the fcc lattice in La${}_{2}B$IrO${}_6$ ($B$ $=$ Mg, Zn)
• Dynamic Jahn-Teller effect in the strong spin-orbit coupling regime
• Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates
• Active role of the nonmagnetic cations in magnetic interactions for the double-perovskite Sr2BOsO6 (B=Y, In, Sc)
• Orbital and spin order in spin-orbit coupled $d^1$ and $d^2$ double perovskites
• Interplay between Spin-Orbit Coupling and Strong Correlation Effects: Comparison of Three Osmate Double Perovskites: Ba${}_{2}A$OsO${}_6$ ($A=$Na, Ca, Y)
• Spin-orbit coupling control of anisotropy, ground state and frustration in 5d2 Sr2MgOsO6
• Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3
• Origin of magnetic excitation gap in double perovskite Sr${}_2$FeOsO${}_6$
• Muon spin rotation and neutron scattering investigations of the B-site ordered double perovskite Sr2DyRuO6
• The role of nonmagnetic d0 vs. d10 B-type cations on the magnetic exchange interactions in osmium double perovskites
• Canted ferrimagnetism and giant coercivity in the non-stoichiometric double perovskite La2Ni1.19Os0.81O6
• Structural and magnetic properties of the 5$d^2$ double perovskites Sr${}_{2}B$ReO${}_6$ ($B$ $=$ Y, In)
• Probing octupolar hidden order via Janus impurities
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• Calculated g-factors of 5d double perovskites Ba2NaOsO6 and Ba2YOsO6
• Osmates on the verge of a Hund's-Mott transition: The different fates of NaOsO${}_3$ and LiOsO${}_3$
• Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6
• Magnon spectrum of the Weyl semimetal half-Heusler compound GdPtBi
• Hidden orders in spin-orbit entangled correlated insulators
• Spin gaps in the ordered states of La${}_2$LiXO${}_6$ (X = Ru, Os) and their relation to distortion of the cubic double perovskite structure in 4$d^3$ and 5$d^3$ magnets
• New Buckled Honeycomb Lattice Compound Sr3CaOs2O9 Exhibiting Antiferromagnetism above Room Temperature
• The complex non-collinear magnetic orderings in Ba2YOsO6: A new approach to tuning spin-lattice interactions and controlling magnetic orderings in frustrated complex oxides
• Effects of the structural distortion on the electronic band structure of {\boldmath $\mathrm{NaOs}{\mathrm{O}}_3$} studied within density functional theory and a three-orbital model
• Magnetically induced metal-insulator transition in Pb2CaOsO6
• Theoretical analysis of single-ion anisotropy in $d^3$ Mott insulators
• Possible origin of the absence of magnetic order in LiOsO${}_3$: Spin-orbit coupling controlled ground state
• Multipolar interactions and magnetic excitation gap in d${}^3$ spin-orbit Mott insulators
• Spin-orbit coupling in a half-filled $t_{2g}$ shell: the case of $5d^3$ K${}_2$ReCl${}_6$
• Magnetic frustration in the cubic double perovskite Ba2NiIrO6
• Neutron Scattering Investigation of Rhenium Orbital Ordering in $3d-5d$ Double Perovskite Ca${}_2$FeReO${}_6$
• Spin-orbit coupling induced magnetic anisotropy and large spin wave gap in $\mathrm{NaOs}{\mathrm{O}}_3$
• Magnetic and electronic properties of La${}_{3}M$O${}_7$ and possible polaron formation in hole-doped La${}_{3}M$O${}_7$ ($M$=Ru and Os)
• Dipolar and quadrupolar correlations in the $5d^2$ Re-based double perovskites Ba${}_2$YReO${}_6$ and Ba${}_2$ScReO${}_6$
• Crystal Growth of a New 8H Perovskite Sr8Os6.3O24 Exhibiting High TC Ferromagnetism