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Register a new userUnified theory of spiral magnetism in the harmonic-honeycomb iridates {alpha}, {beta}, {gamma} Li2IrO3
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A family of insulating iridates with chemical formula Li$_2$IrO$_3$ has recently been discovered, featuring three distinct crystal structures $alpha,beta,gamma$ (honeycomb, hyperhoneycomb, stripyhoneycomb). Measurements on the three-dimensional polytypes, $beta$- and $gamma$-Li$_2$IrO$_3$, found that they magnetically order into remarkably similar spiral phases, exhibiting a non-coplanar counter-rotating spiral magnetic order with equivalent q=0.57 wavevectors. We examine magnetic Hamiltonians for this family and show that the same triplet of nearest-neighbor Kitaev-Heisenberg-Ising (KJI) interactions reproduces this spiral order on both $beta,gamma$-Li$_2$IrO$_3$ structures. We analyze the origin of this phenomenon by studying the model on a 1D zigzag chain, a structural unit common to the three polytypes. The zigzag-chain solution transparently shows how the Kitaev interaction stabilizes the counter-rotating spiral, which is shown to persist on restoring the inter-chain coupling. Our minimal model makes a concrete prediction for the magnetic order in $alpha$-Li$_2$IrO$_3$.
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The realization of Kitaev spin liquid, where spins on a honeycomb lattice are coupled ferromagnetically by bond-dependent anisotropic interactions, has been a sought-after dream. 5d iridium oxides $alpha$-Li2IrO3 and $alpha$-Na2IrO3 with a honeycomb lattice of Jeff = 1/2 moments recently emerged as a possible materialization. Strong signature of Kitaev physics, however, was not captured. Here we report the discovery of a complex iridium oxide $beta$-Li2IrO3 with Jeff = 1/2 moments on hyper-honeycomb lattice, a three-dimensional analogue of honeycomb lattice. A positive Curie-Weiss temperature $theta_{CW}$ ~ 40 K indicated dominant ferromagnetic interactions among Jeff = 1/2 moments in $beta$-Li2IrO3. A magnetic ordering with a small entropy change was observed at Tc = 38 K, which, with the application of magnetic field of only 3 T, changed to a fully polarized state of Jeff = 1/2 moments. Those results imply that hyper-honeycomb beta-Li2IrO3 is located in the vicinity to a Kitaev spin liquid.
The fractionalization of elementary excitations in quantum spin systems is a central theme in current condensed matter physics. The Kitaev honeycomb spin model provides a prominent example of exotic fractionalized quasiparticles, composed of itinerant Majorana fermions and gapped gauge fluxes. However, identification of the Majorana fermions in a three-dimensional honeycomb lattice remains elusive. Here we report spectroscopic signatures of fractional excitations in the harmonic-honeycomb iridates $beta$- and $gamma$-Li$_2$IrO$_3$. Using polarization resolved Raman spectroscopy, we find that the dynamical Raman response of $beta$- and $gamma$-Li$_2$IrO$_3$ features a broad scattering continuum with distinct polarization and composition dependence. The temperature dependence of the Raman spectral weight is dominated by the thermal damping of fermionic excitations. These results suggest the emergence of Majorana fermions from spin fractionalization in a three-dimensional Kitaev-Heisenberg system.
We report the successful synthesis of single-crystals of the layered iridate, (Na$_{1-x}$Li$_{x}$)$_2$IrO$_3$, $0leq x leq 0.9$, and a thorough study of its structural, magnetic, thermal and transport properties. The new compound allows a controlled interpolation between Na$_2$IrO$_3$ and Li$_2$IrO$_3$, while maintaing the novel quantum magnetism of the honeycomb Ir$^{4+}$ planes. The measured phase diagram demonstrates a dramatic suppression of the Neel temperature, $T_N$, at intermediate $x$ suggesting that the magnetic order in Na$_2$IrO$_3$ and Li$_2$IrO$_3$ are distinct, and that at $xapprox 0.7$, the compound is close to a magnetically disordered phase that has been sought after in Na$_2$IrO$_3$ and Li$_2$IrO$_3$. By analyzing our magnetic data with a simple theoretical model we also show that the trigonal splitting, on the Ir$^{4+}$ ions changes sign from Na$_2$IrO$_3$ and Li$_2$IrO$_3$, and the honeycomb iridates are in the strong spin-orbit coupling regime, controlled by $jeff=1/2$ moments.
Honeycomb iridates are thought to have strongly spin-anisotropic exchange interactions that could lead to an extraordinary state of matter known as the Kitaev quantum spin liquid. The realization of this state requires almost perfectly frustrated interactions between the magnetic Ir$^{4+}$ ions, but small imbalances in energy make other ordered states more favorable. Indeed, the closeness in energy of these ordered states is itself a signature of the intrinsic frustration in the system. In this work, we illustrate that small magnetic fields can be employed to drive the frustrated quantum magnet $beta-$Li$_2$IrO$_3$,between different broken symmetry states, but without causing a true thermodynamic phase transition. This field-induced broken symmetry phase has all the signatures of a thermodynamic order parameter, but it is never truly formed in zero field. Rather, it is summoned when the scales of frustration are appropriately tipped, intertwined with other nearby quantum states.
Single-crystal x-ray diffraction studies with synchrotron radiation on the honeycomb iridate $alpha$-Li$_{2}$IrO$_{3}$ reveal a pressure-induced structural phase transition with symmetry lowering from monoclinic to triclinic at a critical pressure of $P_{c}$ = 3.8 GPa. According to the evolution of the lattice parameters with pressure, the transition mainly affects the $ab$ plane and thereby the Ir hexagon network, leading to the formation of Ir--Ir dimers. These observations are independently predicted and corroborated by our textit{ab initio} density functional theory calculations where we find that the appearance of Ir--Ir dimers at finite pressure is a consequence of a subtle interplay between magnetism, correlation, spin-orbit coupling, and covalent bonding. Our results further suggest that at $P_{c}$ the system undergoes a magnetic collapse. Finally we provide a general picture of competing interactions for the honeycomb lattices $A_{2}$$M$O$_{3}$ with $A$= Li, Na and $M$ = Ir, Ru.
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