The monoclinic crystal structure of $\alpha$-RuCl${}_3$ and the zigzag antiferromagnetic ground state

Abstract

The layered honeycomb magnet alpha-RuCl3 has been proposed as a candidate to realize a Kitaev spin model with strongly frustrated, bond-dependent, anisotropic interactions between spin-orbit entangled jeff=1/2 Ru4+ magnetic moments. Here we report a detailed study of the three-dimensional crystal structure using x-ray diffraction on untwinned crystals combined with structural relaxation calculations. We consider several models for the stacking of honeycomb layers and find evidence for a crystal structure with a monoclinic unit cell corresponding to a stacking of layers with a unidirectional in-plane offset, with occasional in-plane sliding stacking faults, in contrast with the currently-assumed trigonal 3-layer stacking periodicity. We report electronic band structure calculations for the monoclinic structure, which find support for the applicability of the jeff=1/2 picture once spin orbit coupling and electron correlations are included. We propose that differences in the magnitude of anisotropic exchange along symmetry inequivalent bonds in the monoclinic cell could provide a natural mechanism to explain the spin gap observed in powder inelastic neutron scattering, in contrast to spin models based on the three-fold symmetric trigonal structure, which predict a gapless spectrum within linear spin wave theory. Our susceptibility measurements on both powders and stacked crystals, as well as neutron powder diffraction show a single magnetic transition at TN ~ 13K. The analysis of the neutron data provides evidence for zigzag magnetic order in the honeycomb layers with an antiferromagnetic stacking between layers. Magnetization measurements on stacked single crystals in pulsed field up to 60T show a single transition around 8T for in-plane fields followed by a gradual, asymptotic approach to magnetization saturation, as characteristic of strongly anisotropic exchange interactions.

13 pages, 9 figures, published in Physical Review B

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• Chemical tuning between triangular and honeycomb structures in a 5$d$ spin-orbit Mott insulator
• Role of disorder in the electronic and magnetic properties of Ag${}_3$LiIr${}_2$O${}_6$
• Intermediate field-induced phase of the honeycomb magnet BaCo${}_2$(AsO${}_4$)${}_2$
• NMR in an electric field: A bulk probe of the hidden spin and orbital polarizations
• Disentangling spin excitation continua in classical and quantum magnets using 2D nonlinear spectroscopy
• Multinode quantum spin liquids in extended Kitaev honeycomb models: the view from variational Monte Carlo
• Anisotropic magnetic interactions in a candidate Kitaev spin liquid close to a metal-insulator transition
• Polarization-dependent magnetic properties of periodically driven $\alpha$-RuCl${}_3$
• Efficient Method for Prediction of Meta-stable/Ground Multipolar Ordered States and its Application in Monolayer $\alpha$-\ce{RuX3} (X=Cl,I)
• Static and fluctuating zigzag order, and possible signatures of Kitaev physics, in torque measurements of $\alpha$-RuCl${}_3$
• Nonsymmorphic bosonization in one-dimensional generalized Kitaev spin-1/2 models
• Giant anisotropic magnetoresistance in few-layer α-RuCl3 tunnel junctions
• Emergent SU(2)${}_1$ conformal symmetry in the spin-1/2 Kitaev-Gamma chain with a Dzyaloshinskii-Moriya interaction
• Unraveling the magnetic ground-state in alkali-metal lanthanide oxide Na${}_2$PrO${}_3$
• Successive topological phase transitions in two distinct spin-flop phases on the honeycomb lattice
• Non-local features of the spin-orbit exciton in Kitaev materials
• Cu-Sb dumbbell arrangement in the spin-orbital liquid candidate Ba${}_3$CuSb${}_2$O${}_9$
• From linear to circular polarized light -- Floquet engineering in Kitaev-Heisenberg materials with Lissajous figures
• Dilution of the magnetic lattice in the Kitaev candidate $\alpha$-RuCl${}_3$ by Rh${}^{3+}$ doping
• Effective Model for Rare-earth Kitaev Materials and its Classical Monte Carlo Simulation
• Thermal Hall conductivity with sign change in the Heisenberg-Kitaev kagome magnet
• High-field quantum spin liquid transitions and angle-field phase diagram of Kitaev magnet $\alpha$-RuCl${}_3$
• Magnetostriction of α-RuCl3 flakes in the zigzag phase
• Signatures of a gapless quantum spin liquid in the Kitaev material Na${}_3$Co${}_{2-x}$Zn${}_x$SbO${}_6$
• Chiral excitations and the intermediate-field spin-liquid regime in the Kitaev magnet $\alpha$-RuCl${}_3$
• Bulk excitations in ultraclean $\alpha$-RuCl${}_3$: Quantitative evidence for Majorana dispersions in a Kitaev quantum spin liquid
• Static and dynamical magnetic properties of the extended Kitaev-Heisenberg model with spin vacancies
• Emergence of bond-dependent highly anisotropic magnetic interactions in Sr${}_4$RhO${}_6$: a theoretical study
• Possible Realization of Kitaev Spin Liquids in van der Waals Heterostructures of $\alpha$-RuCl${}_3$ and Cr$X_3$ ($X$=Cl and I)
• Evidence for distortion-induced local electric polarization in $\alpha$-RuCl${}_3$
• Low-energy spin dynamics in a Kitaev material Na3Ni2BiO6 investigated by NMR
• Nonreciprocal heat transport in the Kitaev chiral spin liquid
• Mott Gap Softening Coinciding with Spin Correlations Collapse in a-RuCl3
• Intermediate phases in $\alpha$-RuCl${}_3$ under in-plane magnetic field via interlayer spin interactions
• Spectrum of the hole excitation in spin-orbit Mott insulator Na${}_2$IrO${}_3$
• Phase diagram for Hole-Doped Kitaev System on the Honeycomb Lattice
• The ground state in a proximity to a possible Kitaev spin liquid: An undistorted honeycomb iridate NaxIrO3 (0.60 < x < 0.80)
• First-principles-based calculation of branching ratio for 5$\mathbf{d}$, 4$\mathbf{d}$, and 3$\mathbf{d}$ transition metal systems
• Bi${}_2$Se${}_3$ thin films heteroepitaxially grown on $\alpha$-RuCl${}_3$
• Field tuning Kitaev systems for spin fractionalization and topological order
• Direct evidence for anisotropic magnetic interaction in $\alpha$-RuCl${}_3$ from polarized inelastic neutron scattering
• Electronic transport mechanisms in a thin crystal of the Kitaev candidate $\alpha$-RuCl${}_3$ probed through guarded high impedance measurements
• Real-time control of non-Abelian anyons in Kitaev spin liquid under energy dissipation
• A primer on Kitaev Model: Basic aspects, material realization, and recent experiments
• Thermal decomposition of the Kitaev material $\alpha$-RuCl${}_3$ and its influence on low-temperature behavior
• The free energy of anisotropic quantum spin systems: Functional integral representation
• Electron spin resonance study on the 4f honeycomb quantum magnet YbCl3
• Coupled spin-1/2 antiferromagnetic chain Cs${}_2$LiRuCl${}_6$ with partially disordered crystal lattice
• Deciphering competing interactions of Kitaev-Heisenberg-$\Gamma$ system in clusters: part I -- static properties
• Spin and Valley Polarized Multiple Fermi Surfaces of α-RuCl${}_3$/Bilayer Graphene Heterostructure
• Ferrichiral skyrmions with sublattice-resolved chirality in extended Kitaev model in triangular lattice
• First-principles study of bulk stacking, $J_{\mathrm{eff}}$ picture, magnetic Hamiltonian, $g$ factors, and structural distortions of $\alpha$-RuCl${}_3$
• Field-induced phase transitions in the Kitaev-Heisenberg model: A sign-problem-free quantum Monte Carlo study and possible application to $\alpha$-RuCl3
• Temperature-dependent magnetic anisotropy from directional-dependent interactions
• Bond disorder in extended Heisenberg-Kitaev models: Spin textures and in-gap states in the high-field regime
• Enhanced Magnetism and Phase Transitions in Ultrathin Quantum Spin Liquid Na2IrO3 Flakes
• Computational exploration of a viable route to Kitaev-quantum spin liquid phase in OsCl${}_3$
• Understanding the magnetic interactions of the zig-zag honeycomb lattice: Application to $\alpha$-RuCl${}_3$
• Magnetodielectric Properties in Two Dimensional Magnetic Insulators
• Robustness of Vacancy-Bound Non-Abelian Anyons in the Kitaev Model in a Magnetic Field
• Magnetostriction in the $J$-$K$-$\Gamma$ model: Application of the numerical linked cluster expansion
• Vortex creation and control in the Kitaev spin liquid by local bond modulations
• Ligand-SOC enhanced $4f^5$ Kitaev antiferromagnet: Application to ${\mathrm{SmI}}_3$
• Nesting instability of gapless U(1) spin liquids with spinon Fermi pockets in two dimensions
• Trigonal distortion in the Kitaev candidate honeycomb magnet BaCo2(AsO4)2
• Tuning the Chern number of Kitaev quantum spin liquid
• Dominant Kitaev Interaction and Field-induced Quantum Disordered Phase in the Cobaltate Na${}_2$Co${}_2$TeO${}_6$
• Ground state of the staggered Heisenberg-$\Gamma$ honeycomb model in a magnetic field
• Low-temperature spin dynamics and absence of magnetic order in layered $\alpha$-RuI${}_3$
• Strategy to Extract Kitaev Interaction using Symmetry in Honeycomb Mott Insulators
• The Role of the Third Dimension in Searching Majorana Fermions in $\alpha$-RuCl${}_3$ via Phonons
• Spin sensitive transport in RuCl_3/Pt heterostructures: revealing a field-transverse spin anisotropy in a spin liquid candidate
• Spin disorder state induced by Mg${}^{2+}$ doping in a Kitaev material Na${}_3$Co${}_2$SbO${}_6$