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Abstract:

We report the synthesis and electronic properties of polycrystalline samples of Zr6MBi2 (M = Ru and Fe) crystallizing in the hexagonal Zr6CoAl2-type structure. Based on their electrical resistivity, magnetization, and heat capacity data, Zr6RuBi2 and Zr6FeBi2 are found to exhibit bulk superconductivity below Tc = 4.9 and 1.4 K, respectively. Although Zr6RuBi2 is most likely a conventional superconductor, the considerably higher Tc for M = Ru compared with that for M = Fe differs from the trend in Tc for Zr6CoAl2-type superconductors reported to date. The superconductivity of an amorphous solid-solution phase, which may hinder elucidation of the superconducting properties of Zr6MBi2, is also discussed.

Abstract:

The physics of spin-orbit entangled magnetic moments of 4d and 5d transition metal ions on a honeycomb lattice has been much explored in search for unconventional magnetic orders or quantum spin liquids expected for compass spin models, where different bonds in the lattice favour different orientations for the magnetic moments. Realizing such physics with rare-earth ions is a promising route to achieve exotic ground states in the extreme spin orbit limit, however this regime has remained experimentally largely unexplored due to major challenges in materials synthesis. Here we report successful synthesis of powders and single crystals of β-Na2PrO3, with Pr^{4+} j_eff = 1/2 magnetic moments arranged on a hyperhoneycomb lattice with the same threefold coordination as the planar honeycomb. We find a strongly noncollinear magnetic order with highly dispersive gapped excitations that we argue arise from frustration between bond-dependent, anisotropic off-diagonal exchanges, a compass quantum spin model not explored experimentally so far. Our results show that rare-earth ions on threefold coordinated lattices offer a platform for the exploration of quantum compass spin models in the extreme spin orbit regime, with qualitatively distinct physics from that of 4d and 5d Kitaev materials.

Abstract:

Rare-earth oxides have attracted interest as a platform for studying frustrated magnetism arising from bond-dependent anisotropic interactions. Ordered rock salt compounds Na₂PrO₃ crystallize in two polymorphs (α and β) comprising honeycomb and hyperhoneycomb lattices of octahedrally coordinated Pr⁴⁺ (4f¹). Although possible realization of antiferromagnetic Kitaev interactions is anticipated for these phases on the basis of ab initio models, the air sensitivity of the two polymorphs has hampered reliable crystal growth and physical property measurements. Here, we have succeeded in preparing powder and single crystals of both α- and β-Na₂PrO₃ using modified synthetic procedures. Revised crystal structures for both polymorphs are obtained from refinement of untwinned single-crystal X-ray diffraction data.