We report the crystal structure, magnetization and neutron scattering measurements on the double perovskite Ba2YOsO6. The F m3m space group is found both at 290 K and 3.5 K with cell constants a0 = 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 θ = −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 ∼ 69 K, is revealed by magnetization, Fisher heat capacity and elastic neutron scattering, with an ordered moment of 1.65(6) µB on Os 5+ . The ordered moment is much reduced from either the expected spin only value of ∼ 3µB or the value appropriate to 4d 3 Ru 5+ in isostructural Ba2YRuO6 of 2.2(1) µB, 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 ∆ ∼ 17 meV, unexpected for an orbitally quenched, d3 electronic configuration. We discuss this in the context of the ∼ 5 meV spin gap observed in the related Ru 5+ , 4d 3 cubic double perovskite Ba2YRuO6, and attribute the ∼ 3 times larger gap to stronger SOC present in this heavier, 5d, osmate system.

Neutron scattering measurements on the pyrochlore magnet Ce2Zr2O7 reveal an unusual crystal field splitting of its lowest J = 5/2 multiplet, such that its ground state doublet is composed of mJ = ± 3/2, giving these doublets a dipole -octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with θCW = -0.4(2) K, leading to a naive expectation of an All-In, All-Out ordered state at low temperatures. Instead our low energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |Q| = 0, and no long range order at low temperatures. This is consistent with recent theory predicting symmetry enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce2Zr2O7 and could play an important role in the low temperature behaviour of this material.The rare-earth pyrochlore oxides R 2 B 2 O 7 , where R 3+ and B 4+ consist generally of rare earth and transitionmetal ions respectively, display a wealth of both exotic and conventional magnetic ground states. Their R 3+ ions decorate a network of corner-sharing tetrahedra, one of the archetypes for geometrical frustration in three dimensions. Due to strong crystal electric field (CEF) effects, the nature of the magnetic interactions in such materials are strongly influenced by their single-ion physics [1][2][3]. A naive theoretical description of the magnetic interactions in rare-earth pyrochlores is generally performed by introducing an ad hoc effective single-ion term in addition to Heisenberg exchange interactions. For example, Heisenberg antiferromagnetism with an effective Ising anisotropy leads to non-frustrated All-In, All-Out (AIAO) magnetic order, as seen in several heavy rare earth iridate pyrochlores [4,5] and illustrated in the insert to Fig.1(a). Heisenberg ferromagnetism and an effective Ising anisotropy give rise to a classical spin ice ground state [6], as seen in (Ho,Dy) 2 Ti 2 O 7 [7, 8] and illustrated as the 2I2O local structure in the inset to Fig.1(a). However, to capture all the physics that can arise at low temperatures, the magnetic interactions should be projected into pseudo-spin operators acting solely on the low energy CEF states [3,[9][10][11][12][13]. This procedure has been applied for example in the Yb 3+ [11,14,15] and Er 3+ [12, 16-18] XY pyrochlores where CEF effects give rise to effective S = 1/2 quantum degrees of freedom that interact via anisotropic exchange interactions.More recently, it has been realized that the precise composition of the ground state crystal field doublets in rare-earth pyrochlores is crucial in determining the form of the microscopic Hamiltonian, and in itself, diversifies the possibility of quantum magnetic states [3,19]. This has been appreciated for some time in the case of non-Kramers doublets, based on magnetic ions with an even number of electrons such as the 4f 2 configuratio...

The geometrically frustrated double perovskite Ba2YRuO6 has magnetic 4d 3 Ru 5+ ions decorating an undistorted face-centered cubic (FCC) lattice. This material has been previously reported to exhibit commensurate long-range antiferromagnetic order below TN ∼ 36 K, a factor f ∼ 15 times lower than its Curie-Weiss temperature ΘCW = −522 K, and purported short-range order to T * = 47 K. We report new time-of-flight neutron spectroscopy of Ba2YRuO6 which shows the development of a ∼5 meV spin gap in the vicinity of the [100] magnetic ordering wavevector below TN =36 K, with the transition to long-range order occurring at T * = 47 K. We also report spin waves extending to ∼14 meV, a surprisingly small bandwidth in light of the large ΘCW . We compare the spin gap and bandwidth to relevant neutron studies of the isostructural 4d 1 material Ba2YMoO6, and discuss the results in the framework of relatively strong spin-orbit coupling expected in 4d magnetic systems.

We report time-of-flight neutron spectroscopic and diffraction studies of the 5d 2 cubic double pervoskite magnets, Ba2M OsO6 (M = Zn, Mg, Ca). These cubic materials are all described by antiferromagnetically-coupled 5d 2 Os 6+ ions decorating a face-centred cubic (FCC) lattice. They all exhibit thermodynamic anomalies consistent with phase transitions at a temperature T * , and exhibit a gapped magnetic excitation spectrum with spectral weight concentrated at wavevectors typical of type I antiferromagnetic orders. While muon spin resonance experiments show clear evidence for time reversal symmetry breaking, no corresponding magnetic Bragg scattering is observed at low temperatures. These results are argued to be consistent with low temperature octupolar order, and are discussed in the context of other 5d DP magnets, and theories for d 2 ions on a FCC lattice which predict exotic orders driven by multipolar interactions.