Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet alpha-RuCl3

Abstract

Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material alpha-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p=0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin liquid phase in alpha-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.

References in corpus (28)

• Anyons in an exactly solved model and beyond
• Proximate Kitaev Quantum Spin Liquid Behaviour in α-RuCl${}_3$
• Neutron tomography of magnetic Majorana fermions in a proximate quantum spin liquid
• Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales
• Low-temperature crystal and magnetic structure of $\alpha$-RuCl3
• Evidence for a Field-induced Quantum Spin Liquid in $\alpha$-RuCl${}_3$
• Excitations in the field-induced quantum spin liquid state of alpha-RuCl3
• Spin-orbit excitation energies, anisotropic exchange, and magnetic phases of honeycomb RuCl3
• Crystal structure and magnetism in $\alpha$-RuCl3: an ab-initio study
• Phase Diagram of $\alpha$-RuCl${}_3$ in an in-plane Magnetic Field
• Anisotropic Ru3+ 4d5 magnetism in the alpha-RuCl3 honeycomb system: susceptibility, specific heat and Zero field NMR
• Anomalous thermal conductivity and magnetic torque response in the honeycomb magnet $\alpha$-RuCl${}_3$
• Large field-induced gap of Kitaev-Heisenberg paramagnons in $\alpha$-RuCl${}_3$
• 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${}_3$
• Magnetization processes of zigzag states on the honeycomb lattice: Identifying spin models for $\alpha$-RuCl${}_3$ and Na${}_2$IrO${}_3$
• Dynamics of Fractionalization in Quantum Spin Liquids
• Probing $\alpha$-RuCl${}_3$ Beyond Magnetic Order: Effects of Temperature and Magnetic Field
• Covalent bonds against magnetism in transition metal compounds
• Antiferromagnetic resonance and terahertz continuum in $\alpha -$RuCl${}_3$
• Ultralow-temperature thermal conductivity of the Kitaev honeycomb magnet $\alpha$-RuCl${}_3$ across the field-induced phase transition
• Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: $\alpha$-Li${}_2$IrO${}_3$ under pressure
• Orbital reconstruction in nonpolar tetravalent transition-metal oxide layers
• High-pressure magnetization and NMR studies on $\alpha$-RuCl${}_3$
• Classical dimers and dimerized superstructure in orbitally degenerate honeycomb antiferromagnet
• Miniature ceramic-anvil high-pressure cell for magnetic measurements in a commercial superconducting quantum interference device magnetometer
• High-temperature magnetostructural transition in van der Waals-layered a-MoCl3
• Dimer phases in quantum antiferromagnets with orbital degeneracy

Cited by in corpus (54)

• Kitaev quantum spin liquid - concept and materialization
• Orbital effects in solids: basics, recent progress and opportunities
• Pressure-tuned magnetic interactions in honeycomb Kitaev materials
• Mott Transition and Superconductivity in Quantum Spin Liquid Candidate NaYbSe${}_2$
• Role of Hydrogen in the spin-orbital-entangled quantum liquid candidate H${}_3$LiIr${}_2$O${}_6$
• Raman evidence for dimerization and Mott collapse in $\alpha$-RuCl${}_3$ under pressures
• Magnetoelastic coupling and effects of uniaxial strain in $\alpha$-RuCl${}_3$ from first principles
• Ground state and low-energy excitations of the Kitaev-Heisenberg ladder
• Phonon renormalization in the Kitaev quantum spin liquid
• Kitaev honeycomb models in magnetic fields: Dynamical response and hidden symmetries
• Pressure-induced collapse of spin-orbital Mott state in the hyperhoneycomb iridate $\beta$-Li${}_2$IrO${}_3$
• Angle-dependent thermodynamics of $\alpha$-RuCl${}_3$
• Collective excitations in the tetravalent lanthanide honeycomb antiferromagnet, Na2PrO3
• Spin-glass state and reversed magnetic anisotropy induced by Cr doping in the Kitaev magnet $\alpha$-RuCl${}_3$
• Investigation of the magnetoelastic coupling anisotropy in the Kitaev material $\alpha$-RuCl${}_3$
• Chemical- and hydrostatic-pressure effects on the Kitaev honeycomb material Na${}_2$IrO${}_3$
• Kitaev magnetism through the prism of lithium iridate
• Bond ordering and phase transitions in Na${}_2$IrO${}_3$ under high pressure
• Pressure-induced structural dimerization in the hyperhoneycomb iridate $\beta$-Li${}_2$IrO${}_3$ at low temperatures
• Uniaxial and hydrostatic pressure effects in alpha-RuCl3 single crystals via thermal-expansion measurements
• Ground-state phase diagram of the Kitaev-Heisenberg model on a kagome lattice
• Optical signature of the pressure-induced dimerization in the honeycomb iridate $\alpha$-Li${}_2$IrO${}_3$
• Evidence for magnetic fractional excitations in a Kitaev quantum-spin-liquid candidate $\alpha$-RuCl${}_3$
• Pressure-induced formation of rhodium zigzag chains in the honeycomb rhodate Li${}_2$RhO${}_3$
• Majorana edge magnetization in the Kitaev honeycomb model
• Symmetry-protected gapless spin liquids on the strained honeycomb lattice
• Interplay of magnetism and dimerization in pressurized Kitaev material $\beta$-Li${}_2$IrO${}_3$
• Large off diagonal exchange couplings and spin liquid states in ${\mathbf{C}}_3$ symmetric iridates
• Hidden spin-orbital order in the Kitaev hyperhoneycomb $\beta$-Li${}_2$IrO${}_3$
• Quantum paramagnetism in the hyperhoneycomb Kitaev magnet $\beta$-ZnIrO${}_3$
• Lattice dynamics and structural transition of the hyperhoneycomb iridate $\beta$-Li${}_2$IrO${}_3$ investigated by high-pressure Raman scattering
• Energy scales in 4f1 delafossite magnets: crystal-field splittings larger than the strength of spin-orbit coupling in KCeO2
• Pressure tuning of structure, magnetic frustration and carrier conduction in Kitaev spin liquid candidate Cu${}_2$IrO${}_3$: X-ray, Raman, magnetic susceptibility, resistivity and first-principles analysis
• Superexchange interactions between spin-orbit-coupled $j\approx 1/2$ ions in oxides with face-sharing ligand octahedra
• Magnon Condensation in Dimerized Antiferromagnets with Spin-Orbit Coupling
• Confinement transition in a Kitaev-like honeycomb model with bond anisotropy
• Hydrostatic pressure effect on Co-based honeycomb magnet BaCo2(AsO4)2
• Can the highly symmetric SU(4) spin-orbital model be realized in alpha-ZrCl3?
• Room temperature relaxometry of single nitrogen-vacancy centers in proximity to $\alpha$-RuCl${}_3$ nanoflakes
• $J_{\mathrm{eff}}$ = 1/2 Hyperoctagon Lattice in Cobalt Oxalate Metal-Organic-Framework
• Magnetic versus nonmagnetic polymorphs of RuBr${}_3$ under pressure
• Dimer Crystallization Induced by Elemental Substitution in the Honeycomb Lattice of Ru1-xOsxCl3
• Crystal-field effects competing with spin-orbit interactions in NaCeO${}_2$
• Pressure-induced transition from Jeff=1/2 to S=1/2 states in CuAl2O4
• Thermal Hall conductivity with sign change in the Heisenberg-Kitaev kagome magnet
• Pressure tuning of competing interactions on a honeycomb lattice
• Dilution of the magnetic lattice in the Kitaev candidate $\alpha$-RuCl${}_3$ by Rh${}^{3+}$ doping
• Pressure-driven switching of magnetism in layered CrCl3
• Hidden covalent insulator and spin excitations in SrRu${}_2$O${}_6$
• Signature of Topological Semimetal in Harmonic-honeycomb ReO3
• First-principles study of bulk stacking, $J_{\mathrm{eff}}$ picture, magnetic Hamiltonian, $g$ factors, and structural distortions of $\alpha$-RuCl${}_3$
• Formation of orbital molecules on a pyrochlore lattice induced by A-O bond covalency
• Nesting instability of gapless U(1) spin liquids with spinon Fermi pockets in two dimensions
• Ground state of the staggered Heisenberg-$\Gamma$ honeycomb model in a magnetic field