Evolution of Magnetism in Single-Crystal Honeycomb Iridates

Abstract

We report the successful synthesis of single-crystals of the layered iridate, (Na${}_{1-x}$Li${}_x$)${}_2$IrO${}_3$, $0\le x\le 0.9$, 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 Néel 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 $x\approx 0.7$, 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.

arXiv commentupdated version with more data

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• First-Principles Study of the Honeycomb-Lattice Iridates Na2IrO3 in the Presence of Strong Spin-Orbit Interaction and Electron Correlations
• The Challenge of Spin-Orbit-Tuned Ground States in Iridates
• Possible Kitaev Quantum Spin Liquid State in 2D Materials with S=3/2
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• Clues and criteria for designing Kitaev spin liquid revealed by thermal and spin excitations of honeycomb iridates Na${}_2$IrO${}_3$
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• Z_2-vortex lattice in the ground state of the triangular Kitaev-Heisenberg model
• Spiral order in the honeycomb iridate Li2IrO3
• Theory of Magnetic Phase Diagrams in Hyperhoneycomb and Harmonic-honeycomb Iridates
• Strongly frustrated triangular spin lattice emerging from triplet dimer formation in honeycomb Li2IrO3
• Unveiling Magnetic Interactions of Ruthenium Trichloride via Constraining Direction of Orbital moments: Potential Routes to Realize Quantum Spin Liquid
• Lattice-Tuned Magnetism of Ru4+(4d4) Ions in Single-Crystals of the Layered Honeycomb Ruthenates: Li2RuO3 and Na2RuO3
• Effect of nonmagnetic dilution in honeycomb lattice iridates Na${}_2$IrO${}_3$ and Li${}_2$IrO${}_3$
• Pressure-tuning of bond-directional exchange interactions and magnetic frustration in hyperhoneycomb iridate $\beta$-$\mathrm{L}{\mathrm{i}}_2\mathrm{Ir}{\mathrm{O}}_3$
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• Thermodynamic and Transport Properties in Disordered Kitaev Models
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• Two iridates, two models, two approaches: a comparative study on magnetism in 3D honeycomb materials
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• Spin-glass state and reversed magnetic anisotropy induced by Cr doping in the Kitaev magnet $\alpha$-RuCl${}_3$
• Thermal Hall signatures of non-Kitaev spin liquids in honeycomb Kitaev materials
• Spin dynamics in the Kitaev model with disorder: Quantum Monte Carlo study of dynamical spin structure factor, magnetic susceptibility, and NMR relaxation rate
• Raman Signatures of Strong Kitaev Exchange Correlations in (Na${}_{1-x}$Li${}_x$)${}_2$IrO${}_3$ : Experiments and Theory
• Structural, electronic, and magnetic properties of nearly-ideal $J_{\mathrm{eff}}$ $=$ 1/2 iridium halides
• Chemical- and hydrostatic-pressure effects on the Kitaev honeycomb material Na${}_2$IrO${}_3$
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• Unconventional magnetism in the spin-orbit driven Mott insulators Ba3MIr2O9 (M=Sc,Y)
• Kitaev Spin Liquid Candidate OsxCl3 Comprised of Honeycomb Nano-Domains
• Resonant inelastic x-ray scattering spectra in the hyperhoneycomb iridate $\beta$-Li${}_2$IrO${}_3$: First principles calculations
• Evolution of Magnetism in the $N{a}_{3-d}N{a}_{1-x}M{g}_{x}I{r}_2{O}_6$ Series of Honeycomb Iridates
• Triplet FFLO Superconductivity in the doped Kitaev-Heisenberg Honeycomb Model
• Strong tuning of magnetism and electronic structure by spin orientation
• Kinetic Ferromagnetism and Topological Magnons of the Hole-Doped Kitaev Spin Liquid
• Multipolar spin liquid in an exactly solvable model for $j_{\mathrm{eff}}=\frac{3}{2}$ moments
• The ground state in a proximity to a possible Kitaev spin liquid: An undistorted honeycomb iridate NaxIrO3 (0.60 < x < 0.80)
• The nature of low-temperature spin-freezing in frustrated Kitaev magnets
• Topological Majorana flat bands in the Kitaev model on a Bishamon-kikko lattice