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Register a new userStatic and dynamic magnetic properties of honeycomb lattice antiferromagnets Na$_{2}M_{2}$TeO$_{6}$, $M$ = Co and Ni
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The magnetic structures and spin dynamics of Na$_{2}$Co$_{2}$TeO$_{6}$ and Na$_{2}$Ni$_{2}$TeO$_{6}$ are investigated by means of elastic and inelastic neutron scattering measurements and the results are discussed in the context of a generalized Kitaev-Heisenberg model on honeycomb lattice with strong spin-orbit coupling. The large number of parameters involved in the Hamiltonian model are evaluated by using an iterative optimization algorithm capable of extracting model solutions and simultaneously estimating their uncertainty. The analyses establish that both Co$^{2+}$ ($d^7$) and Ni$^{2+}$ ($d^8$) antiferromagnets realize bond-dependent anisotropic nearest-neighbor interactions, and support the theoretical predictions for the realization of Kitaev physics in 3$d$ electron systems with effective spins $S$=1/2 and $S$=1. Furthermore, by studying the Na-doped system Na$_{2.4}$Ni$_{2}$TeO$_{6}$, we show that the control of Na content can provide an effective route for fine tuning the magnetic lattice dimensionality, as well as to controlling the bond-dependent anisotropic interactions.
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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.
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.
We present the results of structural and magnetic phase comparisons of the iron oxychalcogenides La$_{2}$O$_{2}$Fe$_{2}$O$M$$_{2}$ ($M$ = S, Se). Elastic neutron scattering reveals that $M$ = S and Se have similar nuclear structures at room and low temperatures. We find that both materials obtain antiferromagnetic ordering at a Neel temperature $T_{N}$ 90.1 $pm$ 0.16 K and 107.2 $pm$ 0.06 K for $M$= Se and S, respectively. The magnetic arrangements of $M$ = S, Se are obtained through Rietveld refinement. We find the order parameter exponent $beta$ to be 0.129 $pm$ 0.006 for $M$ = Se and 0.133 $pm$ 0.007 for $M$ = S. Each of these values is near the Ising symmetry value of 1/8. This suggests that although lattice and electronic structural modifications result from chalcogen exchange, the nature of the magnetic interactions is similar in these materials.
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.
We have synthesized and characterized different stable phases of sodium cobaltates Na$_{x}$CoO$_{2}$ with sodium content $0.65<x<0.80$. We demonstrate that $^{23}$Na NMR allows to determine the difference in the susceptibility of the phases and reveals the presence of Na order in each phase. $^{59}$Co NMR experiments give clear evidence that Co charge disproportionation is a dominant feature of Na cobaltates. Only a small fraction ($approx$ 25%) of cobalts are in a non-magnetic Co$^{3+}$ charge state whereas electrons delocalize on the other cobalts. The magnetic and charge properties of the different Co sites are highly correlated with each other as their magnetic shift $K_{ZZ}$ scales linearly with their quadrupolar frequency $nu_Q$. This reflects the fact that the hole content on the Co orbitals varies from site to site. The unusual charge differentiation found in this system calls for better theoretical understanding of the incidence of the Na atomic order on the electronic structures of these compounds.
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