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Register a new userMagnetic and electronic ordering phenomena in the [Ru$_2$O$_6$] honeycomb lattice compound AgRuO$_3$
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The silver ruthenium oxide AgRuO$_3$ consists of honeycomb [Ru$_2^{5+}$O$_6^{2-}$] layers, and can be considered an analogue of SrRu$_2$O$_6$ with a different intercalation stage. We present measurements of magnetic susceptibility and specific heat on AgRuO$_3$ single crystals which reveal a sharp antiferromagnetic transition at 342(3)K. The electrical transport in single crystals of AgRuO$_3$ is determined by a combination of activated conduction over an intrinsic semiconducting gap of $approx$ 100 meV and carriers trapped and thermally released from defects. From powder neutron diffraction data a Neel-type antiferromagnetic structure with the Ru moments along the $c$ axis is derived. Raman and muon spin rotation spectroscopy measurements on AgRuO$_3$ powder samples indicate a further weak phase transition or a crossover in the temperature range 125-200 K. The transition does not show up in magnetic susceptibility and its origin is argued to be related to defects but cannot be fully clarified. The experimental findings are complemented by DFT-based electronic structure calculations. It is found that the magnetism in AgRuO$_3$ is similar to that of SrRu$_2$O$_6$, however with stronger intralayer and weaker interlayer magnetic exchange interactions.
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We use x-ray spectroscopy at Ir L$_3$/L$_2$ absorption edge to study powder samples of the intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including next-neighbour Ir-Ir electron hoping integrals, we argue that the intercalation of Ag atoms results in a nearly itinerant electronic structure with enhanced Ir-O hybridization. As a result of the departure from the local relativistic $j_{rm eff}! = !1/2$ state, we find that the relative orbital contribution to the magnetic moment is increased, and the magnetization density is spatially extended and asymmetric. Our results confirm the importance of metal - ligand hybridazation in the magnetism of transition metal oxides and provide empirical guidance for understanding the collective magnetism in intercalated honeycomb iridates.
The high temperature magnetic order in SrRu$_2$O$_6$ was studied by measuring magnetization and neutron powder diffraction with both polarized and unpolarized neutrons. SrRu$_2$O$_6$ crystallizes into the hexagonal lead antimonate (PbSb$_2$O$_6$, space group textit{P}$overline{3}$1textit{m}) structure with layers of edge-sharing RuO$_6$ octahedra separated by Sr$^{2+}$ ions. SrRu$_2$O$_6$ orders at $T_N$=565,K with Ru moments coupled antiferromagnetically both in-plane and out-of-plane. The magnetic moment is 1.30(2) $mu_mathrm{B}$/Ru at room temperature and is along the crystallographic textit{c}-axis in the G-type magnetic structure. We performed density functional calculations with constrained RPA to obtain the electronic structure and effective intra- and inter-orbital interaction parameters. The projected density of states show strong hybridization between Ru 4$d$ and O 2$p$. By downfolding to the target $t_{2g}$ bands we extracted the effective magnetic Hamiltonian. We performed Monte Carlo simulations to determine the transition temperature as a function of inter- and intra-plane couplings and find weak inter plane coupling, 3% of the intra-plane coupling, permits three dimensional magnetic order at $T_N$. As suggested by the magnetic susceptibility, two-dimensional correlations persist above $T_N$ due to the strong intra-plane coupling.
We investigate the structural and magnetic properties of a Kitaev spin liquid candidate material Ag$_3$LiIr$_2$O$_6$ based on $^7$Li nuclear magnetic resonance line shape, Knight shift and spin-lattice relaxation rate $1/T_1$. The first sample A shows signatures of magnetically ordered spins, and exhibits one sharp $^7$Li peak with FWHM increasing significantly below 14~K. $1/T_1^{stretch}$ of this sample displays a broad local maximum at 40~K, followed by a very sharp peak at $T_N = 9pm1$~K due to critical slowing down of Ir spin fluctuations, a typical signature of magnetic long range order. In order to shed light on the position-by-position variation of $1/T_1$ throughout the sample, we use Inverse Laplace Transform $T_1$ analysis based on Tikhonov regularization to deduce the density distribution function $P(1/T_1)$. We demonstrate that $sim 60%$ of Ir spins are statically ordered at the NMR measurement timescale but the rest of the sample volume remains paramagnetic even at 4.2~K, presumably because of structural disorder induced primarily by stacking faults. In order to further investigate the influence of structural disorder, we compare these NMR results with those of a second sample B, which has been shown by transmission electron microscope to have domains with unwanted Ag inclusion at Li and Ir sites within the Ir honeycomb planes. The sample B displays an additional NMR peak with relative intensity of $sim 17%$. The small Knight shift and $1/T_1$ of these defect-induced $^7$Li sites and the enhancement of bulk susceptibility at low temperatures suggest that these defects generate domains of only weakly magnetic Ir spins accompanied by free spins, leading to a lack of clear signatures of long-range order. The apparent lack of long-range order could be easily misinterpreted as evidence for the realization of a spin liquid ground state in highly disordered Kitaev lattice.
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.
Kitaevs honeycomb spin-liquid model and its proposed realization in materials such as $alpha$-RuCl$_3$, Li$_2$IrO$_3$ and Na$_2$IrO$_3$ continue to present open questions about how the dynamics of a spin-liquid are modified in the presence of non-Kitaev interactions as well as the presence of inhomogeneities. Here we use $^{23}$Na nuclear magnetic resonance to probe both static and dynamical magnetic properties in single crystal Na$_2$IrO$_3$. We find that the NMR shift follows the bulk susceptibility above 30 K but deviates from it below; moreover below $T_N$ the spectra show a broad distribution of internal magnetic fields. Both of these results provide evidence for inequivalent magnetic sites at low temperature, suggesting inhomogeneities are important for the magnetism. The spin-lattice relaxation rate is isotropic and diverges at $T_N$, suggesting that the Kitaev cubic axes may control the critical quantum spin fluctuations. In the ordered state, we observe gapless excitations, which may arise from site substitution, emergent defects from milder disorder, or possibly be associated with nearby quantum paramagnetic states distinct from the Kitaev spin liquid.
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