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Abstract:

We report high-resolution inelastic neutron scattering measurements of the excitation spectrum in large single crystals of the spin-1/2 triangular-lattice Ising-like antiferromagnet ${\mathrm{Na}}_2\mathrm{BaCo}{\left({\mathrm{PO}}_4\right)}_2$ in magnetic fields applied transverse to the Ising axis. In the high-field polarized phase above a critical field $B_{\mathrm{C}}$ , we observe sharp magnons, as expected in the case of no exchange disorder. Through simultaneous fits to the dispersions including data in a polarizing field along the Ising axis, we obtain an excellent match to an Ising-like XXZ Hamiltonian and rule out previously proposed Kitaev exchanges. In the intermediate-field phase below $B_{\mathrm{C}}$ , we observe three dispersive modes, out of which only the lowest energy one is sharp and the others are broad and overlap with continuum scattering. We propose that the broadening effects are due to magnon decays into two-magnon excitations and confirm that such processes are kinematically allowed. The continuum scattering becomes progressively stronger upon lowering the field and, at 0.25 T and zero field, it dominates the entire spectrum with no clear evidence for even broadened magnon modes. We discuss the relevance of the continuous manifold of mean-field degenerate ground states of the refined Hamiltonian for capturing the observed spectrum in zero field, and compare the data with the one- and two-magnon spectrum averaged over this manifold. We also propose a model of the interlayer couplings to explain the observed finite interlayer magnetic propagation vector of the zero-field magnetic order; this requires the breaking of the mirror symmetry in the nominal $P\overline{3}m1$ space group and through refinement of x-ray diffraction data on an untwinned single crystal, we indeed confirm a rotation of the ${\mathrm{CoO}}_6$ octahedra around the $c$ axis, which lowers the symmetry to $P\overline{3}$ .

Abstract:

Through a combination of crystal symmetry analysis and density functional theory calculations we unveil a possible microscopic origin of the unexpected insulating behavior reported in the honeycomb Kitaev material Cu₂⁢I����₃. Our study suggests that this material hosts an instability towards charge ordering of the Ir ions, with alternating magnetic Ir⁴⁺ and nonmagnetic Ir³⁺ ions arranged on the honeycomb lattice. In this case, the next-nearest-neighbor interactions that couple magnetic Ir⁴⁺ ions form an enlarged triangular lattice, instead of the expected honeycomb lattice. The magnetic Cu²⁺ ions located at the center of the iridium honeycomb voids also form a triangular lattice, and additionally contribute to the magnetization of the system. Together, the interpenetrated Ir⁴⁺ and Cu²⁺ triangular lattices present a novel type of honeycomb Kitaev lattice composed of two types of magnetic ion.

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:

Kitaev materials often order magnetically at low temperatures due to the presence of non-Kitaev interactions. Torque magnetometry is a very sensitive technique for probing the magnetic anisotropy, which is critical in understanding the magnetic ground state. In this work, we report detailed single-crystal torque measurements in the proposed Kitaev candidate honeycomb magnet α-RuBr3, which displays zigzag order below 34 K. Based on angular-dependent torque studies in magnetic fields up to 16 T rotated in the plane normal to the honeycomb layers, we find an easy-plane anisotropy with a temperature dependence of the torque amplitude following closely the behaviour of the powder magnetic susceptibility. The torque for field rotated in the honeycomb plane has a clear six-fold periodicity with a saw-tooth shape, reflecting the three-fold symmetry of the crystal structure and stabilization of different zigzag domains depending on the field orientation, with a torque amplitude that follows an order parameter form inside the zigzag phase. By comparing experimental data with theoretical calculations we highlight the importance of relevant anisotropic interactions and the role of the competition between different zigzag domains in this candidate Kitaev magnet.