Unconventional magnetic order on the hyperhoneycomb Kitaev lattice in β\beta-Li2IrO3: full solution via magnetic resonant x-ray diffraction

The recently-synthesized iridate $\beta$-Li$_2$IrO$_3$ has been proposed as a candidate to display novel magnetic behavior stabilized by frustration effects from bond-dependent, anisotropic interactions (Kitaev model) on a three-dimensional "hyperhoneycomb" lattice. Here we report a combined study using neutron powder diffraction and magnetic resonant x-ray diffraction to solve the complete magnetic structure. We find a complex, incommensurate magnetic order with non-coplanar and counter-rotating Ir moments, which surprisingly shares many of its features with the related structural polytype "stripyhoneycomb" $\gamma$-Li$_2$IrO$_3$, where dominant Kitaev interactions have been invoked to explain the stability of the observed magnetic structure. The similarities of behavior between those two structural polytypes, which have different global lattice topologies but the same local connectivity, is strongly suggestive that the same magnetic interactions and the same underlying mechanism governs the stability of the magnetic order in both materials, indicating that both $\beta$- and $\gamma$-Li$_2$IrO$_3$ are strong candidates to realize dominant Kitaev interactions in a solid state material.Comment: 14 pages, 9 figure

Effect of isoelectronic doping on honeycomb lattice iridate A_2IrO_3

We have investigated experimentally and theoretically the series (Na$_{1-x}$Li$_{x}$)$_{2}$IrO$_{3}$. Contrary to what has been believed so far, only for $x\leq0.25$ the system forms uniform solid solutions. For larger Li content, as evidenced by powder X-ray diffraction, scanning electron microscopy and density functional theory calculations, the system shows a miscibility gap and a phase separation into an ordered Na$_{3}$LiIr$_2$O$_{6}$ phase with alternating Na$_3$ and LiIr$_2$O$_6$ planes, and a Li-rich phase close to pure Li$_{2}$IrO$_{3}$. For $x\leq 0.25$ we observe (1) an increase of $c/a$ with Li doping up to $x=0.25$, despite the fact that $c/a$ in pure Li$_{2}$IrO$_{3}$ is smaller than in Na$_{2}$IrO$_{3}$, and (2) a gradual reduction of the antiferromagnetic ordering temperature $T_{N}$ and ordered moment. The previously proposed magnetic quantum phase transition at $x\approx 0.7$ may occur in a multiphase region and its nature needs to be re-evaluated.Comment: 8 pages, 9 figures including supplemental informatio

Kitaev interactions between j=1/2 moments in honeycomb Na2IrO3 are large and ferromagnetic: insights from ab initio quantum chemistry calculations

Na$_2$IrO$_3$, a honeycomb 5$d^5$ oxide, has been recently identified as a potential realization of the Kitaev spin lattice. The basic feature of this spin model is that for each of the three metal-metal links emerging out of a metal site, the Kitaev interaction connects only spin components perpendicular to the plaquette defined by the magnetic ions and two bridging ligands. The fact that reciprocally orthogonal spin components are coupled along the three different links leads to strong frustration effects and nontrivial physics. While the experiments indicate zigzag antiferromagnetic order in Na$_2$IrO$_3$, the signs and relative strengths of the Kitaev and Heisenberg interactions are still under debate. Herein we report results of ab initio many-body electronic structure calculations and establish that the nearest-neighbor exchange is strongly anisotropic with a dominant ferromagnetic Kitaev part, whereas the Heisenberg contribution is significantly weaker and antiferromagnetic. The calculations further reveal a strong sensitivity to tiny structural details such as the bond angles. In addition to the large spin-orbit interactions, this strong dependence on distortions of the Ir$_2$O$_2$ plaquettes singles out the honeycomb 5$d^5$ oxides as a new playground for the realization of unconventional magnetic ground states and excitations in extended systems.Comment: 13 pages, 2 tables, 3 figures, accepted in NJ

Spectral signatures of a unique charge density wave in Ta2_2NiSe7_7

Charge Density Waves (CDW) are commonly associated with the presence of near-Fermi level states which are separated from others, or "nested", by a wavector of $\mathbf{q}$. Here we use Angle-Resolved Photo Emission Spectroscopy (ARPES) on the CDW material Ta$_2$NiSe$_7$ and identify a total absence of any plausible nesting of states at the primary CDW wavevector $\mathbf{q}$. Nevertheless we observe spectral intensity on replicas of the hole-like valence bands, shifted by a wavevector of $\mathbf{q}$, which appears with the CDW transition. In contrast, we find that there is a possible nesting at $\mathbf{2q}$, and associate the characters of these bands with the reported atomic modulations at $\mathbf{2q}$. Our comprehensive electronic structure perspective shows that the CDW-like transition of Ta$_2$NiSe$_7$ is unique, with the primary wavevector $\mathbf{q}$ being unrelated to any low-energy states, but suggests that the reported modulation at $\mathbf{2q}$, which would plausibly connect low-energy states, might be more important for the overall energetics of the problem

One-ninth magnetization plateau stabilized by spin entanglement in a kagome antiferromagnet

The spin-1/2 antiferromagnetic Heisenberg model on a Kagome lattice is geometrically frustrated, which is expected to promote the formation of many-body quantum entangled states. The most sought-after among these is the quantum spin liquid phase, but magnetic analogs of liquid, solid, and supersolid phases may also occur, producing fractional plateaus in the magnetization. Here, we investigate the experimental realization of these predicted phases in the Kagome material YCu3(OD)6+xBr3-x (x=0.5). By combining thermodynamic and Raman spectroscopic techniques, we provide evidence for fractionalized spinon excitations and observe the emergence of a 1/9 magnetization plateau. These observations establish YCu3(OD)6+xBr3-x as a model material for exploring the 1/9 plateau phase.Comment: to appear in Nature Physics, 33 pagses, 15 figure