Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3

Laurell, Pontus; Okamoto, Satoshi

doi:10.1038/s41535-019-0203-y

Title: Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3

Abstract

Abstract What is the correct low-energy spin Hamiltonian description of $$$$\alpha$$$$ $α$ -RuCl $$$$_{3}$$$$ $_{3}$ ? The material is a promising Kitaev spin liquid candidate, but is also known to order magnetically, the description of which necessitates additional interaction terms. The nature of these interactions, their magnitudes and even signs, remain an open question. In this work we systematically investigate dynamical and thermodynamic magnetic properties of proposed effective Hamiltonians. We calculate zero-temperature inelastic neutron scattering (INS) intensities using exact diagonalization, and magnetic specific heat using a thermal pure quantum states method. We find that no single current model satisfactorily explains all observed phenomena of $$$$\alpha$$$$ $α$ -RuCl $$$$_{3}$$$$ $_{3}$ . 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.

Authors:

;

Publication Date:: Fri Jan 10 00:00:00 EST 2020

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR). Scientific Discovery through Advanced Computing (SciDAC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

OSTI Identifier:: 1619734

Alternate Identifier(s):: OSTI ID: 1606952

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Published Article

Journal Name:: npj Quantum Materials

Additional Journal Information:: Journal Name: npj Quantum Materials Journal Volume: 5 Journal Issue: 1; Journal ID: ISSN 2397-4648

Publisher:: Nature Publishing Group

Country of Publication:: United Kingdom

Language:: English

Subject:: 36 MATERIALS SCIENCE; Magnetic properties and materials; Quantum fluids and solids

Citation Formats


                    Laurell, Pontus, and Okamoto, Satoshi. Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3.  United Kingdom: N. p., 2020. 
Web.  doi:10.1038/s41535-019-0203-y.

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                    Laurell, Pontus, & Okamoto, Satoshi. Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3.  United Kingdom.  https://doi.org/10.1038/s41535-019-0203-y

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                    Laurell, Pontus, and Okamoto, Satoshi. Fri .  
"Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3".  United Kingdom.  https://doi.org/10.1038/s41535-019-0203-y.

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@article{osti_1619734,

  title        = {Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3},

  author       = {Laurell, Pontus and Okamoto, Satoshi},

  abstractNote = {Abstract What is the correct low-energy spin Hamiltonian description of $$\alpha$$ α -RuCl $$_{3}$$ 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 $$\alpha$$ α -RuCl $$_{3}$$ 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.},

  doi          = {10.1038/s41535-019-0203-y},

  journal      = {npj Quantum Materials},

  number       = 1,

  volume       = 5,

  place        = {United Kingdom},

  year         = {Fri Jan 10 00:00:00 EST 2020},

  month        = {Fri Jan 10 00:00:00 EST 2020}

}

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Title: Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3

Abstract

Citation Formats

Breakdown of magnons in a strongly spin-orbital coupled magnet journal, October 2017

Field-induced quantum criticality in the Kitaev system α − RuCl 3 journal, July 2017

Optical probe of Heisenberg-Kitaev magnetism in α − RuCl 3 journal, November 2016

Quantum lattice model solver H Φ journal, August 2017

Incommensurate counterrotating magnetic order stabilized by Kitaev interactions in the layered honeycomb α − Li 2 IrO 3 journal, May 2016

Erratum: Effective model with strong Kitaev interactions for α − RuCl 3 [Phys. Rev. B 97 , 134424 (2018)] journal, June 2019

2D proximate quantum spin liquid state in atomic-thin α -RuCl 3 journal, November 2018

Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales journal, June 2016

Excitations in the field-induced quantum spin liquid state of α-RuCl3 journal, February 2018

Finite field regime for a quantum spin liquid in α − RuCl 3 journal, August 2019

Phase diagram of α − RuCl 3 in an in-plane magnetic field journal, May 2017

Observation of two types of fractional excitation in the Kitaev honeycomb magnet journal, May 2018

Quantum spin liquids: a review journal, November 2016

Electronically highly cubic conditions for Ru in α − RuCl 3 journal, October 2017

Thermodynamic evidence of fractionalized excitations in α − RuC l 3 journal, March 2019

Quantum spin liquid states journal, April 2017

Models and materials for generalized Kitaev magnetism journal, November 2017

Evidence for a Field-Induced Quantum Spin Liquid in α - RuCl 3 journal, July 2017

Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of α − RuCl 3 journal, December 2017

Successive magnetic phase transitions in α − RuCl 3 : XY-like frustrated magnet on the honeycomb lattice journal, March 2015

Spin-wave analysis of the low-temperature thermal Hall effect in the candidate Kitaev spin liquid α − RuCl 3 journal, August 2018

Anisotropic Ru 3 + 4 d 5 magnetism in the α − RuCl 3 honeycomb system: Susceptibility, specific heat, and zero-field NMR journal, May 2015

Scattering Continuum and Possible Fractionalized Excitations in α − RuCl 3 journal, April 2015

Vaporization of Kitaev Spin Liquids journal, November 2014

α − RuCl 3 : A spin-orbit assisted Mott insulator on a honeycomb lattice journal, July 2014

Unveiling magnetic interactions of ruthenium trichloride via constraining direction of orbital moments: Potential routes to realize a quantum spin liquid journal, August 2017

Colloquium : Herbertsmithite and the search for the quantum spin liquid journal, December 2016

Thermal Pure Quantum States at Finite Temperature journal, June 2012

Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides A 2 IrO 3 journal, July 2010

Crystal structure and magnetism in α − RuCl 3 : An ab initio study journal, April 2016

Theoretical investigation of magnetic dynamics in α − RuCl 3 journal, September 2017

Low-temperature crystal and magnetic structure of α − RuCl 3 journal, April 2016

Specific heat and magnetization study on single crystals of the frustrated quasi-one-dimensional oxide Ca 3 Co 2 O 6 journal, July 2003

Terahertz excitations in α − RuC l 3 : Majorana fermions and rigid-plane shear and compression modes journal, September 2019

Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet journal, April 2016

Spin liquids in frustrated magnets journal, March 2010

Anyons in an exactly solved model and beyond journal, January 2006

Concept and realization of Kitaev quantum spin liquids journal, March 2019

Monoclinic crystal structure of α − RuCl 3 and the zigzag antiferromagnetic ground state journal, December 2015

Path to stable quantum spin liquids in spin-orbit coupled correlated materials journal, April 2018

Anisotropic susceptibilities in the honeycomb Kitaev system α − RuCl 3 journal, September 2018

Magnetic order in α − RuCl 3 : A honeycomb-lattice quantum magnet with strong spin-orbit coupling journal, April 2015

Orbital Order and Fluctuations in Mott Insulators journal, January 2005

Dynamical spin structure factors of α-RuCl 3 journal, March 2018

Physics of the Kitaev Model: Fractionalization, Dynamic Correlations, and Material Connections journal, March 2018

Neutron scattering in the proximate quantum spin liquid α-RuCl 3 journal, June 2017

Magnetic thermal conductivity far above the Néel temperature in the Kitaev-magnet candidate α − RuCl 3 journal, June 2017

Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid journal, July 2018

Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit journal, February 2014

Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models journal, February 2019

Spin Waves and Revised Crystal Structure of Honeycomb Iridate Na 2 IrO 3 journal, March 2012

Correlated electrons in high-temperature superconductors journal, July 1994

Majorana fermions in the Kitaev quantum spin system α-RuCl3 journal, September 2017

Kitaev magnetism in honeycomb RuCl 3 with intermediate spin-orbit coupling journal, June 2015

Magnetic anisotropy in the Kitaev model systems Na 2 IrO 3 and RuCl 3 journal, August 2016

Non-Abelian anyons and topological quantum computation journal, September 2008

Fault-tolerant quantum computation by anyons journal, January 2003

Magnetization processes of zigzag states on the honeycomb lattice: Identifying spin models for α − RuCl 3 and Na 2 IrO 3 journal, August 2017

Direct evidence of a zigzag spin-chain structure in the honeycomb lattice: A neutron and x-ray diffraction investigation of single-crystal Na 2 IrO 3 journal, May 2012

Theory of the field-revealed Kitaev spin liquid journal, June 2019

Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models journal, January 2009

Long-range magnetic ordering in Na 2 IrO 3 journal, June 2011

Thermal fractionalization of quantum spins in a Kitaev model: Temperature-linear specific heat and coherent transport of Majorana fermions journal, September 2015

Spin-Wave Excitations Evidencing the Kitaev Interaction in Single Crystalline α − RuCl 3 journal, March 2017

Clues and criteria for designing a Kitaev spin liquid revealed by thermal and spin excitations of the honeycomb iridate Na 2 IrO 3 journal, May 2016

Breakdown of magnons in a strongly spin-orbital coupled magnet
journal, October 2017

Field-induced quantum criticality in the Kitaev system $α - {RuCl}_{3}$
journal, July 2017

Optical probe of Heisenberg-Kitaev magnetism in $α − {RuCl}_{3}$
journal, November 2016

Quantum lattice model solver $H Φ$
journal, August 2017

Incommensurate counterrotating magnetic order stabilized by Kitaev interactions in the layered honeycomb $α − {Li}_{2} {IrO}_{3}$
journal, May 2016

Erratum: Effective model with strong Kitaev interactions for $α − {RuCl}_{3}$ [Phys. Rev. B 97 , 134424 (2018)]
journal, June 2019

2D proximate quantum spin liquid state in atomic-thin α -RuCl ₃
journal, November 2018

Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales
journal, June 2016

Excitations in the field-induced quantum spin liquid state of α-RuCl3
journal, February 2018

Finite field regime for a quantum spin liquid in $α − {RuCl}_{3}$
journal, August 2019

Phase diagram of $α - {RuCl}_{3}$ in an in-plane magnetic field
journal, May 2017

Observation of two types of fractional excitation in the Kitaev honeycomb magnet
journal, May 2018

Quantum spin liquids: a review
journal, November 2016

Electronically highly cubic conditions for Ru in $α - {RuCl}_{3}$
journal, October 2017

Thermodynamic evidence of fractionalized excitations in $α - RuC l_{3}$
journal, March 2019

Quantum spin liquid states
journal, April 2017

Models and materials for generalized Kitaev magnetism
journal, November 2017

Evidence for a Field-Induced Quantum Spin Liquid in $α$ - ${RuCl}_{3}$
journal, July 2017

Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of $α − {RuCl}_{3}$
journal, December 2017

Successive magnetic phase transitions in $α - {RuCl}_{3}$ : XY-like frustrated magnet on the honeycomb lattice
journal, March 2015

Spin-wave analysis of the low-temperature thermal Hall effect in the candidate Kitaev spin liquid $α - {RuCl}_{3}$
journal, August 2018

Anisotropic ${Ru}^{3 +} 4 d^{5}$ magnetism in the $α - {RuCl}_{3}$ honeycomb system: Susceptibility, specific heat, and zero-field NMR
journal, May 2015

Scattering Continuum and Possible Fractionalized Excitations in $α − {RuCl}_{3}$
journal, April 2015

Vaporization of Kitaev Spin Liquids
journal, November 2014

$α - {RuCl}_{3}$ : A spin-orbit assisted Mott insulator on a honeycomb lattice
journal, July 2014

Unveiling magnetic interactions of ruthenium trichloride via constraining direction of orbital moments: Potential routes to realize a quantum spin liquid
journal, August 2017

Colloquium : Herbertsmithite and the search for the quantum spin liquid
journal, December 2016

Thermal Pure Quantum States at Finite Temperature
journal, June 2012

Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides $A_{2} {IrO}_{3}$
journal, July 2010

Crystal structure and magnetism in $α - {RuCl}_{3}$ : An ab initio study
journal, April 2016

Theoretical investigation of magnetic dynamics in $α - {RuCl}_{3}$
journal, September 2017

Low-temperature crystal and magnetic structure of $α - {RuCl}_{3}$
journal, April 2016

Specific heat and magnetization study on single crystals of the frustrated quasi-one-dimensional oxide ${Ca}_{3} {Co}_{2} O_{6}$
journal, July 2003

Terahertz excitations in $α − RuC l_{3}$ : Majorana fermions and rigid-plane shear and compression modes
journal, September 2019

Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016

Spin liquids in frustrated magnets
journal, March 2010

Anyons in an exactly solved model and beyond
journal, January 2006

Concept and realization of Kitaev quantum spin liquids
journal, March 2019

Monoclinic crystal structure of $α - {RuCl}_{3}$ and the zigzag antiferromagnetic ground state
journal, December 2015

Path to stable quantum spin liquids in spin-orbit coupled correlated materials
journal, April 2018

Anisotropic susceptibilities in the honeycomb Kitaev system $α - {RuCl}_{3}$
journal, September 2018

Magnetic order in $α - {RuCl}_{3}$ : A honeycomb-lattice quantum magnet with strong spin-orbit coupling
journal, April 2015

Orbital Order and Fluctuations in Mott Insulators
journal, January 2005

Dynamical spin structure factors of α-RuCl ₃
journal, March 2018

Physics of the Kitaev Model: Fractionalization, Dynamic Correlations, and Material Connections
journal, March 2018

Neutron scattering in the proximate quantum spin liquid α-RuCl ₃
journal, June 2017

Magnetic thermal conductivity far above the Néel temperature in the Kitaev-magnet candidate $α − {RuCl}_{3}$
journal, June 2017

Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid
journal, July 2018

Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit
journal, February 2014

Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models
journal, February 2019

Spin Waves and Revised Crystal Structure of Honeycomb Iridate ${Na}_{2} {IrO}_{3}$
journal, March 2012

Correlated electrons in high-temperature superconductors
journal, July 1994

Majorana fermions in the Kitaev quantum spin system α-RuCl3
journal, September 2017

Kitaev magnetism in honeycomb ${RuCl}_{3}$ with intermediate spin-orbit coupling
journal, June 2015

Magnetic anisotropy in the Kitaev model systems ${Na}_{2} {IrO}_{3}$ and ${RuCl}_{3}$
journal, August 2016

Non-Abelian anyons and topological quantum computation
journal, September 2008

Fault-tolerant quantum computation by anyons
journal, January 2003

Magnetization processes of zigzag states on the honeycomb lattice: Identifying spin models for $α − {RuCl}_{3}$ and ${Na}_{2} {IrO}_{3}$
journal, August 2017

Direct evidence of a zigzag spin-chain structure in the honeycomb lattice: A neutron and x-ray diffraction investigation of single-crystal Na $_{2}$ IrO $_{3}$
journal, May 2012

Theory of the field-revealed Kitaev spin liquid
journal, June 2019

Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009

Long-range magnetic ordering in Na $_{2}$ IrO $_{3}$
journal, June 2011

Thermal fractionalization of quantum spins in a Kitaev model: Temperature-linear specific heat and coherent transport of Majorana fermions
journal, September 2015

Spin-Wave Excitations Evidencing the Kitaev Interaction in Single Crystalline $α − {RuCl}_{3}$
journal, March 2017

Clues and criteria for designing a Kitaev spin liquid revealed by thermal and spin excitations of the honeycomb iridate ${Na}_{2} {IrO}_{3}$
journal, May 2016