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Register a new userMagnetic anisotropy of the alkali iridate Na$_{2}$IrO$_{3}$ at high magnetic fields: evidence for strong ferromagnetic Kitaev correlations
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The magnetic field response of the Mott-insulating honeycomb iridate Na$_{2}$IrO$_{3}$ is investigated using torque magnetometry measurements in magnetic fields up to 60 tesla. A peak-dip structure is observed in the torque response at magnetic fields corresponding to an energy scale close to the zigzag ordering ($approx 15~K$) temperature. Using exact diagonalization calculations, we show that such a distinctive signature in the torque response constrains the effective spin models for these classes of Kitaev materials to ones with dominant ferromagnetic Kitaev interactions, while alternative models with dominant antiferromagnetic Kitaev interactions are excluded. We further show that at high magnetic fields, long range spin correlation functions decay rapidly, signaling a transition to a long-sought-after field-induced quantum spin liquid beyond the peak-dip structure. Kitaev systems are thus revealed to be excellent candidates for field-induced quantum spin liquids, similar physics having been suggested in another Kitaev material $alpha-$RuCl$_{3}$.
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Temperature-pressure phase diagram of the Kitaev hyperhoneycomb iridate $beta$-Li$_2$IrO$_3$ is explored using magnetization, thermal expansion, magnetostriction, and muon spin rotation ($mu$SR) measurements, as well as single-crystal x-ray diffraction under pressure and ab initio calculations. The Neel temperature of $beta$-Li$_2$IrO$_3$ increases with the slope of 0.9 K/GPa upon initial compression, but the reduction in the polarization field $H_c$ reflects a growing instability of the incommensurate order. At 1.4 GPa, the ordered state breaks down upon a first-order transition giving way to a new ground state marked by the coexistence of dynamically correlated and frozen spins. This partial freezing in the absence of any conspicuous structural defects may indicate classical nature of the resulting pressure-induced spin liquid, an observation paralleled to the increase in the nearest-neighbor off-diagonal exchange $Gamma$ under pressure.
In RuCl$_3$, inelastic neutron scattering and Raman spectroscopy reveal a continuum of non-spin-wave excitations that persists to high temperature, suggesting the presence of a spin liquid state on a honeycomb lattice. In the context of the Kitaev model, magnetic fields introduce finite interactions between the elementary excitations, and thus the effects of high magnetic fields - comparable to the spin exchange energy scale - must be explored. Here we report measurements of the magnetotropic coefficient - the second derivative of the free energy with respect to magnetic field orientation - over a wide range of magnetic fields and temperatures. We find that magnetic field and temperature compete to determine the magnetic response in a way that is independent of the large intrinsic exchange interaction energy. This emergent scale-invariant magnetic anisotropy provides evidence for a high degree of exchange frustration that favors the formation of a spin liquid state in RuCl$_3$.
We study the effect of isoelectronic doping and external pressure in tuning the ground state of the honeycomb iridate Na$_2$IrO$_3$ by combining optical spectroscopy with synchrotron x-ray diffraction measurements on single crystals. The obtained optical conductivity of Na$_2$IrO$_3$ is discussed in terms of a Mott insulating picture versus the formation of quasimolecular orbitals and in terms of Kitaev-interactions. With increasing Li content $x$, (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ moves deeper into the Mott insulating regime and there are indications that up to a doping level of 24% the compound comes closer to the Kitaev-limit. The optical conductivity spectrum of single crystalline $alpha$-Li$_2$IrO$_3$ does not follow the trends observed for the series up to $x=0.24$. There are strong indications that $alpha$-Li$_2$IrO$_3$ is less close to the Kitaev-limit compared to Na$_2$IrO$_3$ and closer to the quasimolecular orbital picture. Except for the pressure-induced hardening of the phonon modes, the optical properties of Na$_2$IrO$_3$ seem to be robust against external pressure. Possible explanations of the unexpected evolution of the optical conductivity with isolectronic doping and the drastic change between $x=0.24$ and $x=1$ are given by comparing the pressure-induced changes of lattice parameters and the optical conductivity with the corresponding changes induced by doping.
$alpha$-RuCl$_3$ is drawing much attention as a promising candidate Kitaev quantum spin liquid. However, despite intensive research efforts, controversy remains about the form of the basic interactions governing the physics of this material. Even the sign of the Kitaev interaction (the bond-dependent anisotropic interaction responsible for Kitaev physics) is still under debate, with conflicting results from theoretical and experimental studies. The significance of the symmetric off-diagonal exchange interaction (referred to as the $Gamma$ term) is another contentious question. Here, we present resonant elastic x-ray scattering data that provides unambiguous experimental constraints to the two leading terms in the magnetic interaction Hamiltonian. We show that the Kitaev interaction ($K$) is ferromagnetic, and that the $Gamma$ term is antiferromagnetic and comparable in size to the Kitaev interaction. Our findings also provide a natural explanation for the large anisotropy of the magnetic susceptibility in $alpha$-RuCl$_3$ as arising from the large $Gamma$ term. We therefore provide a crucial foundation for understanding the interactions underpinning the exotic magnetic behaviours observed in $alpha$-RuCl$_3$.
Direct experimental investigations of the low-energy electronic structure of the Na$_2$IrO$_3$ iridate insulator are sparse and draw two conflicting pictures. One relies on flat bands and a clear gap, the other involves dispersive states approaching the Fermi level, pointing to surface metallicity. Here, by a combination of angle-resolved photoemission, photoemission electron microscopy, and x-ray absorption, we show that the correct picture is more complex and involves an anomalous band, arising from charge transfer from Na atoms to Ir-derived states. Bulk quasiparticles do exist, but in one of the two possible surface terminations the charge transfer is smaller and they remain elusive.
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