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Register a new userSpin waves and revised crystal structure of honeycomb iridate Na2IrO3
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We report inelastic neutron scattering measurements on Na2IrO3, a candidate for the Kitaev spin model on the honeycomb lattice. We observe spin-wave excitations below 5 meV with a dispersion that can be accounted for by including substantial further-neighbor exchanges that stabilize zig-zag magnetic order. The onset of long-range magnetic order below 15.3 K is confirmed via the observation of oscillations in zero-field muon-spin rotation experiments. Combining single-crystal diffraction and density functional calculations we propose a revised crystal structure model with significant departures from the ideal 90 deg Ir-O-Ir bonds required for dominant Kitaev exchange.
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Heisenberg interactions are ubiquitous in magnetic materials and have been prevailing in modeling and designing quantum magnets. Bond-directional interactions offer a novel alternative to Heisenberg exchange and provide the building blocks of the Kitaev model, which has a quantum spin liquid (QSL) as its exact ground state. Honeycomb iridates, A2IrO3 (A=Na,Li), offer potential realizations of the Kitaev model, and their reported magnetic behaviors may be interpreted within the Kitaev framework. However, the extent of their relevance to the Kitaev model remains unclear, as evidence for bond-directional interactions remains indirect or conjectural. Here, we present direct evidence for dominant bond-directional interactions in antiferromagnetic Na2IrO3 and show that they lead to strong magnetic frustration. Diffuse magnetic x-ray scattering reveals broken spin-rotational symmetry even above Neel temperature, with the three spin components exhibiting nano-scale correlations along distinct crystallographic directions. This spin-space and real-space entanglement directly manifests the bond-directional interactions, provides the missing link to Kitaev physics in honeycomb iridates, and establishes a new design strategy toward frustrated magnetism.
We propose a theoretical model for a gapless spin liquid phase that may have been observed in a recent experiment on $mathrm{H_3Li Ir_2 O_6}$. Despite the insulating and non-magnetic nature of the material, the specific heat coefficient $C/T sim 1/sqrt{T}$ in zero magnetic field and $C/T sim T/ B^{3/2}$ with finite magnetic field $B$ have been observed. In addition, the NMR relaxation rate shows $1/(T_1T) sim (C/T)^2$. Motivated by the fact that the interlayer/in-plane lattice parameters are reduced/elongated by the hydrogen-intercalation of the parent compound $mathrm{Li_2 Ir O_3}$, we consider four layers of the Kitaev honeycomb lattice model with additional interlayer exchange interactions. It is shown that the resulting spin liquid excitations reside mostly in the top and bottom layers of such a layered structure and possess a quartic dispersion. In an applied magnetic field, each quartic mode is split into four Majorana cones with the velocity $v sim B^{3/4}$. We suggest that the spin liquid phase in these defect layers, placed between different stacking patterns of the honeycomb layers, can explain the major phenomenology of the experiment, which can be taken as evidence that the Kitaev interaction plays the primary role in the formation of a quantum spin liquid in this material.
Honeycomb iridate Na2IrO3, a Jeff=1/2 magnet, is a potential platform for realizing the quantum spin liquid. Many experiments have shown that its magnetic ground state has a zigzag antiferromagnetic (AFM) order. However, there is still a lack of consensus on the theoretical model explaining such order, since its second nearest neighbor (NN) and long-range third NN magnetic interactions are highly unclear. By properly taking into account the orbital moments, achieved through constraining their directions in the first-principles calculations, we obtain that the relative angle between orbital and spin moments is fairly small and in the order of several degrees, which thus validates the Jeff=1/2 state in Na2IrO3. Surprisingly, we find that the long-range third NN Heisenberg interactions are sizable whereas the second NN magnetic interactions are negligible. Using maximally localized Wannier functions, we show that the sizable long-range third NN Heisenberg interaction results from the extended nature of the Jeff=1/2 state. Based on our study, we propose a minimal J1-K1-{Gamma}_1-J3 model in which the magnetic excitations have an intensity peak at 5.6 meV, consistent with the inelastic neutron scattering experiment [Phys. Rev. Lett. 108, 127204 (2012)]. The present work demonstrates again that constraining orbital moments in the first-principles calculations is powerful to investigate the intriguing magnetism in the Jeff=1/2 magnets, and paves the way toward gaining a deep insight into the novel magnetism discovered in the honeycomb Jeff=1/2 magnets.
The physics of Mott insulators underlies diverse phenomena ranging from high temperature superconductivity to exotic magnetism. Although both the electron spin and the structure of the local orbitals play a key role in this physics, in most systems these are connected only indirectly --- via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) open a further dimension to this problem by introducing strong spin-orbit interactions, such that the Mott physics has a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin-anisotropic interactions, coupling the spin orientation to a given spatial direction of exchange and leading to strongly frustrated magnetism. The potential for new physics emerging from such interactions has driven much scientific excitement, most recently in the search for a new quantum spin liquid, first discussed by Kitaev cite{kitaev_anyons_2006}. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb, but in a three-dimensional framework. The temperature dependence of the magnetic susceptibility exhibits a striking reordering of the magnetic anisotropy, giving evidence for highly spin-anisotropic exchange interactions. Furthermore, the basic structural units of this material suggest the possibility of a new family of structures, the `harmonic honeycomb iridates. This compound thus provides a unique and exciting glimpse into the physics of a new class of strongly spin-orbit coupled Mott insulators.
We use neutron scattering to study the spin and lattice structure on single crystals of SrFe2As2, the parent compound of the FeAs based superconductor (Sr,K)Fe2As2. We find that SrFe2As2 exhibits an abrupt structural phase transitions at 220K, where the structure changes from tetragonal with lattice parameters c > a = b to orthorhombic with c > a > b. At almost the same temperature, Fe spins in SrFe2As2 develop a collinear antiferromagnetic structure along the orthorhombic a-axis with spin direction parallel to this a-axis. These results are consistent with earlier work on the RFeAsO (R = rare earth elements) families of materials and on BaFe2As2, and therefore suggest that static antiferromagnetic order is ubiquitous for the parent compound of these FeAs-based high-transition temperature superconductors.
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