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Register a new userResonant x-ray scattering reveals possible disappearance of magnetic order under hydrostatic pressure in the Kitaev candidate $gamma$-Li$_2$IrO$_3$
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Honeycomb iridates such as $gamma$-Li$_2$IrO$_3$ are argued to realize Kitaev spin-anisotropic magnetic exchange, along with Heisenberg and possibly other couplings. While systems with pure Kitaev interactions are candidates to realize a quantum spin liquid ground state, in $gamma$-Li$_2$IrO$_3$ it has been shown that the balance of magnetic interactions leads to the incommensurate spiral spin order at ambient pressure below 38 K. We study the fragility of this state in single crystals of $gamma$-Li$_2$IrO$_3$ using resonant x-ray scattering (RXS) under applied hydrostatic pressures of up to 3.0 GPa. RXS is a direct probe of the underlying electronic order, and we observe the abrupt disappearance of the $q$=(0.57, 0, 0) spiral order at a critical pressure $P_c = 1.5 $GPa with no accompanying change in the symmetry of the lattice. This dramatic disappearance is in stark contrast with recent studies of $beta$-Li$_2$IrO$_3$ that show continuous suppression of the spiral order in magnetic field; under pressure, a new and possibly nonmagnetic ground state emerges.
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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.
We present magnetization measurements on polycrystalline $beta$-Li$_2$IrO$_3$ under hydrostatic pressures up to 3 GPa and construct the temperature-pressure phase diagram of this material. The magnetically ordered phase with $T_{rm{N}}simeq 38$ K breaks down upon a pressure-induced first-order phase transition at $p_{rm{c}}$ $approx$ 1.4 GPa and gives way to a high-pressure phase, where a step-like feature in the magnetic susceptibility signals a structural dimerization with a loss of Ir$^{4+}$ magnetic moments. Nevertheless, magnetism manifests itself also above $p_{rm{c}}$ via the Curie-like susceptibility upturn with the effective moment of 0.7 $mu_B$. We suggest that a partially dimerized phase with a mixture of the magnetic and non-magnetic Ir$^{4+}$ sites develops above $p_{rm{c}}$. This phase is thermodynamically stable between 1.7 and 2.7 GPa according to our ab initio calculations. It confines the magnetic Ir$^{4+}$ sites to weakly coupled tetramers with the singlet ground state and no long-range magnetic order. Our results rule out the formation of a pressure-induced spin-liquid phase in $beta$-Li$_2$IrO$_3$ and reveal peculiarities of the magnetism collapse transition in a Kitaev material.
We report the existence of a phase transition at high temperature in the 3D Kitaev candidate material, $beta$-Li$_2$IrO$_3$. We show that the transition is bulk, intrinsic and orders a tiny magnetic moment with a spatially anisotropic saturation moment. We show that even though this transition is global, it does not freeze the local Ir moments, which order at much lower temperatures into an incommensurate state. Rather, the ordered moment has an orbital origin that is coupled to spin correlations, likely of a Kitaev origin. The separate ordering of spin-correlated orbital moments and of local Ir moments reveals a novel way in which magnetic frustration in Kitaev systems can lead to coexisting magnetic states.
The low-temperature magnetic properties of tcr{polycrystalline} Na$_2$IrO$_3$, a candidate material for the realization of a quantum spin-liquid state, were investigated by means of muon-spin relaxation and nuclear magnetic resonance methods under chemical and hydrostatic pressure. The Li-for-Na chemical substitution promotes an inhomogeneous magnetic order, whereas hydrostatic pressure (up to 3.9,GPa) results in an enhancement of the ordering temperature $T_mathrm{N}$. In the first case, the inhomogeneous magnetic order suggests either short- or long-range correlations of broadly distributed $j=,$textonehalf Ir$^{4+}$ magnetic moments, reflecting local disorder. The increase of $T_mathrm{N}$ under applied pressure points at an increased strength of three dimensional interactions arising from interlayer compression.
The magnetic structure of honeycomb iridate Na$_2$IrO$_3$ is of paramount importance to its exotic properties. The magnetic order is established experimentally to be zigzag antiferromagnetic. However, the previous assignment of ordered moment to the $bm{a}$-axis is tentative. We examine the magnetic structure of Na$_{2}$IrO$_{3}$ using first-principles methods. Our calculations reveal that total energy is minimized when the zigzag antiferromagnetic order is magnetized along $bm{g}approxbm{a}+bm{c}$. Such a magnetic configuration is explained by adding anisotropic interactions to the nearest-neighbor Kitaev-Heisenberg model. Spin-wave spectrum is also calculated, where the calculated spin gap of $10.4$ meV can in principle be measured by future inelastic neutron scattering experiments. Finally we emphasize that our proposal is consistent with all known experimental evidence, including the most relevant resonant x-ray magnetic scattering measurements [X. Liu emph{et al.} {Phys. Rev. B} textbf{83}, 220403(R) (2011)].
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