Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate $\alpha$-RuCl${}_3$

Abstract

What is the correct low-energy spin Hamiltonian description of $\alpha$-RuCl${}_3$? The material is a promising Kitaev spin liquid candidate, but is also known to order magnetically, the description of which necessitates additional interaction terms. The nature of these interactions, their magnitudes and even signs, remain an open question. In this work we systematically investigate dynamical and thermodynamic magnetic properties of proposed effective Hamiltonians. We calculate zero-temperature inelastic neutron scattering (INS) intensities using exact diagonalization, and magnetic specific heat using a thermal pure quantum states method. We find that no single current model satisfactorily explains all observed phenomena of $\alpha$-RuCl${}_3$. In particular, we find that Hamiltonians derived from first principles can capture the experimentally observed high-temperature peak in the magnetic specific heat, while overestimating the magnon energy at the zone center. In contrast, other models reproduce important features of the INS data, but do not adequately describe the magnetic specific heat. To address this discrepancy we propose a modified ab initio model that is consistent with both magnetic specific heat and low-energy features of INS data.

arXiv commentMain text: 12 pages, 8 figures. Supplemental Information: 16 pages, 18 figures

References in corpus (70)

• Fault-tolerant quantum computation by anyons
• Non-Abelian Anyons and Topological Quantum Computation
• Anyons in an exactly solved model and beyond
• Correlated Electrons in High Temperature Superconductors
• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• Quantum Spin Liquids
• Quantum Spin Liquid States
• Kitaev-Heisenberg Model on Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides $A_2$IrO${}_3$
• Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid
• Kitaev quantum spin liquid - concept and materialization
• $\alpha$-RuCl3: a Spin-Orbit Assisted Mott Insulator on a Honeycomb Lattice
• Neutron tomography of magnetic Majorana fermions in a proximate quantum spin liquid
• Generic spin model for the honeycomb iridates beyond the Kitaev limit
• Models and Materials for Generalized Kitaev Magnetism
• Spin waves and revised crystal structure of honeycomb iridate Na2IrO3
• Herbertsmithite and the Search for the Quantum Spin Liquid
• Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales
• The monoclinic crystal structure of $\alpha$-RuCl${}_3$ and the zigzag antiferromagnetic ground state
• Scattering Continuum and Possible Fractionalized Excitations in $\alpha$-RuCl${}_3$
• Magnetic order in $\alpha$-RuCl${}_3$: a honeycomb lattice quantum magnet with strong spin-orbit coupling
• Physics of the Kitaev model: fractionalization, dynamical correlations, and material connections
• Orbital order and fluctuations in Mott insulators
• Low-temperature crystal and magnetic structure of $\alpha$-RuCl3
• Direct evidence of a zigzag spin chain structure in the honeycomb lattice: A neutron and x-ray diffraction investigation on single crystal $\mathrm{N}{\mathrm{a}}_2\mathrm{Ir}{\mathrm{O}}_3$
• Evidence for a Field-induced Quantum Spin Liquid in $\alpha$-RuCl${}_3$
• Dynamics of a two-dimensional quantum spin liquid: signatures of emergent Majorana fermions and fluxes
• Excitations in the field-induced quantum spin liquid state of alpha-RuCl3
• Long range magnetic ordering in Na${}_2$IrO${}_3$
• Successive magnetic phase transitions in $\mathbf{\alpha }$-RuCl${}_3$: XY-like frustrated magnet on the honeycomb lattice
• Kitaev magnetism in honeycomb RuCl3 with intermediate spin-orbit coupling
• Breakdown of Magnons in a Strongly Spin-Orbital Coupled Magnet
• Crystal structure and magnetism in $\alpha$-RuCl3: an ab-initio study
• Phase Diagram of $\alpha$-RuCl${}_3$ in an in-plane Magnetic Field
• Thermal fractionalization of quantum spins in a Kitaev model: $T$-linear specific heat and coherent transport of Majorana fermions
• Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of alpha-RuCl3
• Spin-wave excitations evidencing the Kitaev interaction in single crystalline $\alpha$-RuCl${}_3$
• Thermal Pure Quantum States at Finite Temperature
• Anisotropic Ru3+ 4d5 magnetism in the alpha-RuCl3 honeycomb system: susceptibility, specific heat and Zero field NMR
• Vaporization of Kitaev spin liquids
• Field-induced quantum criticality in the Kitaev system $\alpha$-RuCl${}_3$
• Magnetic Excitations and Continuum of a Field-Induced Quantum Spin Liquid in $\alpha$-RuCl${}_3$
• Incommensurate Counterrotating Magnetic Order Stabilized by Kitaev Interactions in the Layered Honeycomb $\alpha$-Li${}_2$IrO${}_3$
• Magnetization processes of zigzag states on the honeycomb lattice: Identifying spin models for $\alpha$-RuCl${}_3$ and Na${}_2$IrO${}_3$
• Probing $\alpha$-RuCl${}_3$ Beyond Magnetic Order: Effects of Temperature and Magnetic Field
• Observation of two types of anyons in the Kitaev honeycomb magnet
• Magnetic anisotropy in the Kitaev model systems Na2IrO3 and RuCl3
• Theoretical investigation of the magnetic dynamics in $\alpha$-RuCl${}_3$
• Specific heat and magnetization study on single crystals of a frustrated, quasi one-dimensional oxide: Ca3Co2O6
• Theory of the field-revealed Kitaev spin liquid
• Finite field regime for a quantum spin liquid in $\alpha$-RuCl${}_3$
• Clues and criteria for designing Kitaev spin liquid revealed by thermal and spin excitations of honeycomb iridates Na${}_2$IrO${}_3$
• Antiferromagnetic resonance and terahertz continuum in $\alpha -$RuCl${}_3$
• Quantum Lattice Model Solver $\mathcal{H}\Phi$
• Anisotropic susceptibilities in the honeycomb Kitaev system $\alpha$-RuCl${}_3$
• Thermodynamic evidence of fractionalized excitations in α-RuCl3
• Spin Wave Analysis of Low-Temperature Thermal Hall Effect in the Candidate Kitaev Spin Liquid $\alpha$-RuCl${}_3$
• Magnetic thermal conductivity far above the Néel temperatures in the Kitaev-magnet candidate $\alpha$-RuCl${}_3$
• Unveiling Magnetic Interactions of Ruthenium Trichloride via Constraining Direction of Orbital moments: Potential Routes to Realize Quantum Spin Liquid
• Path to stable quantum spin liquids in spin-orbit coupled correlated materials
• Field evolution of magnons in $\alpha$-RuCl${}_3$ by high-resolution polarized terahertz spectroscopy
• Impact of off-diagonal exchange interactions on the Kitaev spin liquid state of $\alpha$-RuCl${}_3$
• Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models
• Signatures of low-energy fractionalized excitations in $\alpha$-RuCl${}_3$ from field-dependent microwave absorption
• Classical and quantum spin dynamics of the honeycomb $\Gamma$ model
• Deriving models for the Kitaev spin-liquid candidate material $\alpha$-RuCl${}_3$ from first principles
• Electronically highly cubic conditions for Ru in alpha-RuCl3
• Effective model with strong Kitaev interactions for $\alpha$-$\mathrm{RuC}{\mathrm{l}}_3$
• Magnetic field-dependent low-energy magnon dynamics in $\alpha$-RuCl3
• THz excitations in α-RuCl3: Majorana fermions, rigid-plane shear and compression modes
• Chiral spin-order in some purported Kitaev spin-liquid compounds

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• Proximate Kitaev system for an intermediate magnetic phase in in-plane magnetic fields
• Spontaneous Chiral-Spin Ordering in Spin-Orbit Coupled Honeycomb Magnets
• Accuracy of the typicality approach using Chebyshev polynomials
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• Orbital Frustration and Emergent Flat Bands
• Probing critical spin fluctuations with a composite magnetoelectric method: A case study on a Kitaev spin liquid candidate Na${}_3$Co${}_2$SbO${}_6$
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• A primer on Kitaev Model: Basic aspects, material realization, and recent experiments
• Direct evidence for anisotropic magnetic interaction in $\alpha$-RuCl${}_3$ from polarized inelastic neutron scattering
• Bond disorder in extended Heisenberg-Kitaev models: Spin textures and in-gap states in the high-field regime
• First-principles study of bulk stacking, $J_{\mathrm{eff}}$ picture, magnetic Hamiltonian, $g$ factors, and structural distortions of $\alpha$-RuCl${}_3$
• Scale-invariant magnetic anisotropy in $\alpha$-RuCl${}_3$: A quantum Monte Carlo study
• Pressure-dependent magnetism of the Kitaev candidate Li${}_2$RhO${}_3$
• Real-space spectral simulation of quantum spin models: Application to generalized Kitaev models
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