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Register a new userSodium layer chiral distribution and spin structure of Na$_2$Ni$_2$TeO$_6$ with a honeycomb network
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The nature of Na ion distribution, diffusion path, and the spin structure of $P2$-type Na$_2$Ni$_2$TeO$_6$ with a Ni honeycomb network has been explored. The nuclear density distribution of Na ions reveals a 2D chiral pattern within Na layers without breaking the original 3D crystal symmetry, which has been achieved uniquely via an inverse Fourier transform (iFT)-assisted neutron diffraction technique. The Na diffusion pathway described by the calculated iso-surface of Na ion bond valence sum (BVS) map is found consistent to a chiral diffusion mechanism. The Na site occupancy and Ni$^{2+}$ spin ordering were examined in detail with the electron density mapping, neutron diffraction, magnetic susceptibility, specific heat, thermal conductivity and transport measurements. Signatures of both strong incommensurate (ICM) and weak commensurate (CM) antiferromagnetic (AFM) spin ordering were identified in the polycrystalline sample studied, and the CM-AFM spin ordering was confirmed by using a single crystal sample through the $k$-scan in the momentum space corresponding to the AFM peak of ($frac{1}{2}$, 0, 1).
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Co$^{2+}$ ions in an octahedral crystal field, stabilise a j$_{eff}$ = 1/2 ground state with an orbital degree of freedom and have been recently put forward for realising Kitaev interactions, a prediction we have tested by investigating spin dynamics in two cobalt honeycomb lattice compounds, Na$_2$Co$_2$TeO$_6$ and Na$_3$Co$_2$SbO$_6$, using inelastic neutron scattering. We used linear spin wave theory to show that the magnetic spectra can be reproduced with a spin Hamiltonian including a dominant Kitaev nearest-neighbour interaction, weaker Heisenberg interactions up to the third neighbour and bond-dependent off-diagonal exchange interactions. Beyond the Kitaev interaction that alone would induce a quantum spin liquid state, the presence of these additional couplings is responsible for the zigzag-type long-range magnetic ordering observed at low temperature in both compounds. These results provide evidence for the realization of Kitaev-type coupling in cobalt-based materials, despite hosting a weaker spin-orbit coupling than their 4d and 5d counterparts.
In the quest of finding novel and efficient batteries, a great interest has raised in K-based honeycomb layer oxide materials both for their fundamental properties and potential applications. A key issue in the realization of efficient batteries based on such compounds, is to understand the K-ion diffusion mechanism. However, investigation of potassium-ion (K$^+$) dynamics in materials using magneto-spin properties has so far been challenging, due to its inherently weak nuclear magnetic moment, in contrast to other alkali ions such as lithium and sodium. Spin-polarised muons, having a high gyromagnetic ratio, make the muon spin rotation and relaxation ($mu$+SR) technique ideal for probing ions dynamics in weak magneto-spin moment materials. Here we report the magnetic properties and K+ dynamics in honeycomb layered oxide material of the K$_2$Ni$_2$TeO$_6$ using $mu$+SR measurements. Our low-temperature $mu$+SR results together with, with complementary magnetic susceptibility, find an antiferromagnetic transition at 26 K. Further $mu$+SR studies performed at higher temperatures reveal that potassium ions (K$^+$) become mobile above 250 K and the activation energy for the diffusion process is Ea = 121(13) meV. This is the first time that K+ dynamics in potassium-based battery materials has been measured using $mu$+SR. Finally our results also indicate an interesting possibility that K-ion self diffusion occurs predominantly at the surface of the powder particles. This opens future possibilities for improving ion diffusion and device performance using nano-structuring.
Finding new materials with antiferromagnetic (AFM) Kitaev interaction is an urgent issue to broaden and enrich the quantum magnetism research significantly. By carrying out inelastic neutron scattering experiments and subsequent analysis, we conclude that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are new honeycomb cobalt-based AFM Kitaev systems. The spin-orbit excitons at 20-28~meV in both compounds strongly supports the idea that Co$^{2+}$ ions of both compounds have a spin-orbital entangled $J_rm{eff}=1/2$ state. Furthermore, we found that a generalized Kitaev-Heisenberg Hamiltonian can well describe the spin-wave excitations of both compounds with additional 3rd nearest-neighbor interaction. Our best-fit parameters show large AFM Kitaev terms and off-diagonal symmetric anisotropy terms of a similar magnitude in both compounds. We should stress that our parameters optimized magnetic structures are consistent with the magnetic structures reported from neutron diffraction studies. Moreover, there is also the magnon-damping effect at the higher energy part of the spin waves, as usually observed in other Kitaev magnets. We demonstrate that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are the first experimental realization of AFM Kitaev magnets based on the systematic studies of the spin waves and analysis.
Spin-1/2 chains with alternating antiferromagnetic (AF) and ferromagnetic (FM) couplings exhibit quantum entanglement like the integer-spin Haldane chains and might be similarly utilized for quantum computations. Such alternating AF-FM chains have been proposed to be realized in the distorted honeycomb-lattice compound Na$_2$Cu$_2$TeO$_6$, but to confirm this picture a comprehensive understanding of the exchange interactions including terms outside of the idealized model is required. Here we employ neutron scattering to study the spin dynamics in Na$_2$Cu$_2$TeO$_6$ and accurately determine the coupling strengths through the random phase approximation and density functional theory (DFT) approaches. We find the AF and FM intrachain couplings are the dominant terms in the spin Hamiltonian, while the interchain couplings are AF but perturbative. This hierarchy in the coupling strengths and the alternating signs of the intrachain couplings can be understood through their different exchange paths. Our results establish Na$_2$Cu$_2$TeO$_6$ as a weakly-coupled alternating AF-FM chain compound and reveal the robustness of the gapped ground state in alternating chains under weak interchain couplings.
Na$_2$Co$_2$TeO$_6$ has recently been proposed to be a Kitaev-like honeycomb magnet. To assess how close it is to realizing Kitaev quantum spin liquids, we have measured magnetization and specific heat on high-quality single crystals in magnetic fields applied along high-symmetry directions. Small training fields reveal a weak but canonical ferrimagnetic behavior below 27 K, which cannot be explained by the zigzag antiferromagnetic order alone and suggests coexisting N{e}el-type order of moments canted away from the zigzag chains. Moderate fields in the honeycomb plane suppress the thermal transition at 27 K, and seem to partly reverse the moment-canting when applied perpendicular to the zigzag chains. In contrast, out-of-plane fields leave the transition largely unaffected, but promotes another transition below 10 K, possibly also related to canting reversal. The magnetism in Na$_2$Co$_2$TeO$_6$ is highly anisotropic and close to tipping points between competing phases.
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