Field evolution of magnons in α-RuCl3 by high-resolution polarized terahertz spectroscopy

Wu, Liang; Little, A.; Aldape, E. E.; Rees, D.; Thewalt, E.; Lampen-Kelley, P.; Banerjee, A.; Bridges, C. A.; Yan, J. -Q.; Boone, D.; Patankar, S.; Goldhaber-Gordon, D.; Mandrus, D.; Nagler, S. E.; Altman, E.; Orenstein, J.

doi:10.1103/physrevb.98.094425

Title: Field evolution of magnons in $α - {RuCl}_{3}$ by high-resolution polarized terahertz spectroscopy

Abstract

The Kitaev quantum spin liquid (KSL) is a theoretically predicted state of matter whose fractionalized quasiparticles are distinct from bosonic magnons, the fundamental excitation in ordered magnets. The layered honeycomb antiferromagnet α-RuCl3 is a KSL candidate material, as it can be driven to a magnetically disordered phase by application of an in-plane magnetic field, with Hc~7T. Here, we report a detailed characterization of the magnetic excitation spectrum of this material by high-resolution time-domain terahertz spectroscopy. We observe two sharp magnon resonances whose frequencies and amplitudes exhibit a discontinuity as a function of applied magnetic field, as well as two broader peaks at higher energy. Below the Néel temperature, we find that linear spin wave theory can account for all of these essential features of the spectra when a C3-breaking distortion of the honeycomb lattice and the presence of structural domains are taken into account.

Authors:

Wu, Liang ^[1]; Little, A. ^[2]; Aldape, E. E. ^[3]; Rees, D. ^[2]; Thewalt, E. ^[2]; Lampen-Kelley, P. ^[4]; Banerjee, A. ^[5]; Bridges, C. A. ^[5]; Yan, J. -Q. ^[5]; Boone, D. ^[6]; Patankar, S. ^[2]; Goldhaber-Gordon, D. ^[6]; Mandrus, D. ^[4]; Nagler, S. E. ^[5]; Altman, E. ^[3]; Orenstein, J. ^[2]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Pennsylvania, Philadelphia, PA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: 2018-09-26

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Gordon and Betty Moore Foundation; USDOE

OSTI Identifier:: 1562881

Alternate Identifier(s):: OSTI ID: 1474001; OSTI ID: 1761765

Grant/Contract Number:: KC2206; AC02-05-CH11231; AC02-05CH11231; AC02-76SF00515; AC05-00OR22725; GBMF4537

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 98; Journal Issue: 9; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Wu, Liang, Little, A., Aldape, E. E., Rees, D., Thewalt, E., Lampen-Kelley, P., Banerjee, A., Bridges, C. A., Yan, J. -Q., Boone, D., Patankar, S., Goldhaber-Gordon, D., Mandrus, D., Nagler, S. E., Altman, E., and Orenstein, J. Field evolution of magnons in α-RuCl3 by high-resolution polarized terahertz spectroscopy.  United States: N. p., 2018. 
Web.  doi:10.1103/physrevb.98.094425.

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                    Wu, Liang, Little, A., Aldape, E. E., Rees, D., Thewalt, E., Lampen-Kelley, P., Banerjee, A., Bridges, C. A., Yan, J. -Q., Boone, D., Patankar, S., Goldhaber-Gordon, D., Mandrus, D., Nagler, S. E., Altman, E., & Orenstein, J. Field evolution of magnons in α-RuCl3 by high-resolution polarized terahertz spectroscopy.  United States.  https://doi.org/10.1103/physrevb.98.094425

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                    Wu, Liang, Little, A., Aldape, E. E., Rees, D., Thewalt, E., Lampen-Kelley, P., Banerjee, A., Bridges, C. A., Yan, J. -Q., Boone, D., Patankar, S., Goldhaber-Gordon, D., Mandrus, D., Nagler, S. E., Altman, E., and Orenstein, J. Wed .  
"Field evolution of magnons in α-RuCl3 by high-resolution polarized terahertz spectroscopy".  United States.  https://doi.org/10.1103/physrevb.98.094425.  https://www.osti.gov/servlets/purl/1562881.

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@article{osti_1562881,

  title        = {Field evolution of magnons in α-RuCl3 by high-resolution polarized terahertz spectroscopy},

  author       = {Wu, Liang and Little, A. and Aldape, E. E. and Rees, D. and Thewalt, E. and Lampen-Kelley, P. and Banerjee, A. and Bridges, C. A. and Yan, J. -Q. and Boone, D. and Patankar, S. and Goldhaber-Gordon, D. and Mandrus, D. and Nagler, S. E. and Altman, E. and Orenstein, J.},

  abstractNote = {The Kitaev quantum spin liquid (KSL) is a theoretically predicted state of matter whose fractionalized quasiparticles are distinct from bosonic magnons, the fundamental excitation in ordered magnets. The layered honeycomb antiferromagnet α-RuCl3 is a KSL candidate material, as it can be driven to a magnetically disordered phase by application of an in-plane magnetic field, with Hc~7T. Here, we report a detailed characterization of the magnetic excitation spectrum of this material by high-resolution time-domain terahertz spectroscopy. We observe two sharp magnon resonances whose frequencies and amplitudes exhibit a discontinuity as a function of applied magnetic field, as well as two broader peaks at higher energy. Below the Néel temperature, we find that linear spin wave theory can account for all of these essential features of the spectra when a C3-breaking distortion of the honeycomb lattice and the presence of structural domains are taken into account.},

  doi          = {10.1103/physrevb.98.094425},

  journal      = {Physical Review B},

  number       = 9,

  volume       = 98,

  place        = {United States},

  year         = {2018},

  month        = {9}

}

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https://doi.org/10.1103/physrevb.98.094425

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Cited by: 34 works

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Figures / Tables:

Fig. 1: (a) Transmitted THz electric eld amplitude at T = 294 K as a function of sample angle. Blue and red lines represent the minimum transmission axes at a' and b' (b) Schematic of honeycomb structure showing a and b monoclinic axes relative to Ru-Ru bonds. Color of atomsmore »

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Works referencing / citing this record:

Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3
journal, January 2020

Laurell, Pontus; Okamoto, Satoshi
npj Quantum Materials, Vol. 5, Issue 1
DOI: 10.1038/s41535-019-0203-y

Concept and realization of Kitaev quantum spin liquids
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Takagi, Hidenori; Takayama, Tomohiro; Jackeli, George
Nature Reviews Physics, Vol. 1, Issue 4
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Kitaev honeycomb models in magnetic fields: Dynamical response and dual models
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Kaib, David A. S.; Winter, Stephen M.; Valentí, Roser
Physical Review B, Vol. 100, Issue 14
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Two-step gap opening across the quantum critical point in the Kitaev honeycomb magnet $α − {RuCl}_{3}$
journal, January 2020

Nagai, Yuya; Jinno, Takaaki; Yoshitake, Junki
Physical Review B, Vol. 101, Issue 2
DOI: 10.1103/physrevb.101.020414

Two-step gap opening across the quantum critical point in a Kitaev honeycomb magnet
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Nagai, Y.; Jinno, T.; Yoshitake, Y.
arXiv
DOI: 10.48550/arxiv.1810.05379

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Title: Field evolution of magnons in α - RuCl 3 by high-resolution polarized terahertz spectroscopy

Abstract

Citation Formats

Figures / Tables:

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

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

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

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

Mechanism for subgap optical conductivity in honeycomb Kitaev materials journal, April 2018

Field Dependence of the Intrinsic Domain Magnetization of a Ferromagnet journal, December 1940

Field-induced magnon excitation and in-gap absorption in the Kitaev candidate RuCl 3 journal, September 2018

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

Probing α − RuCl 3 Beyond Magnetic Order: Effects of Temperature and Magnetic Field journal, February 2018

Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in γ − Li 2 IrO 3 journal, November 2014

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

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

Ultralow-Temperature Thermal Conductivity of the Kitaev Honeycomb Magnet α − RuCl 3 across the Field-Induced Phase Transition journal, February 2018

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

Antiferromagnetic Resonance and Terahertz Continuum in α − RuCl 3 journal, November 2017

Magnetic Excitations and Continuum of a Possibly Field-Induced Quantum Spin Liquid in α − RuCl 3 journal, November 2017

Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3 journal, November 2016

Linear spin wave theory for single-Q incommensurate magnetic structures journal, March 2015

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

Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate journal, June 2014

Unconventional spin dynamics in the honeycomb-lattice material α − RuCl 3 : High-field electron spin resonance studies journal, December 2017

Effective model with strong Kitaev interactions for α − RuCl 3 journal, April 2018

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

Electronic and phonon excitations in α − RuC l 3 journal, October 2017

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

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

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

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

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

Hyperhoneycomb Iridate β − Li 2 IrO 3 as a Platform for Kitaev Magnetism journal, February 2015

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

Unusual Phonon Heat Transport in α − RuCl 3 : Strong Spin-Phonon Scattering and Field-Induced Spin Gap journal, March 2018

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

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

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

Diagonalization of the quadratic boson hamiltonian journal, September 1978

Relation between Kitaev magnetism and structure in α − RuCl 3 journal, May 2017

Anomalous Thermal Conductivity and Magnetic Torque Response in the Honeycomb Magnet α − RuCl 3 journal, May 2017

Fault-tolerant quantum computation by anyons journal, January 2003

Emergent phenomena induced by spin–orbit coupling at surfaces and interfaces journal, November 2016

Scanning X-ray microdiffraction with submicrometer white beam for strain/stress and orientation mapping in thin films journal, February 2003

Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3 journal, December 2016

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

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 journal, May 2015

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

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

Excitations in the field-induced quantum spin liquid state of α-RuCl3 text, January 2018

Generic spin model for the honeycomb iridates beyond the Kitaev limit text, January 2013

Linear spin wave theory for single-Q incommensurate magnetic structures text, January 2014

Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales text, January 2016

Mechanism for subgap optical conductivity in honeycomb Kitaev materials text, January 2017

Anyons in an exactly solved model and beyond text, January 2005

Fault-tolerant quantum computation by anyons text, January 1997

Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3 journal, January 2020

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

Kitaev honeycomb models in magnetic fields: Dynamical response and dual models journal, October 2019

Two-step gap opening across the quantum critical point in the Kitaev honeycomb magnet α − RuCl 3 journal, January 2020

Two-step gap opening across the quantum critical point in a Kitaev honeycomb magnet text, January 2018

Title: Field evolution of magnons in $α - {RuCl}_{3}$ by high-resolution polarized terahertz spectroscopy

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

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

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

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

Mechanism for subgap optical conductivity in honeycomb Kitaev materials
journal, April 2018

Field Dependence of the Intrinsic Domain Magnetization of a Ferromagnet
journal, December 1940

Field-induced magnon excitation and in-gap absorption in the Kitaev candidate ${RuCl}_{3}$
journal, September 2018

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

Probing $α - {RuCl}_{3}$ Beyond Magnetic Order: Effects of Temperature and Magnetic Field
journal, February 2018

Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in $γ − {Li}_{2} {IrO}_{3}$
journal, November 2014

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

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

Ultralow-Temperature Thermal Conductivity of the Kitaev Honeycomb Magnet $α − {RuCl}_{3}$ across the Field-Induced Phase Transition
journal, February 2018

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

Antiferromagnetic Resonance and Terahertz Continuum in $α − {RuCl}_{3}$
journal, November 2017

Magnetic Excitations and Continuum of a Possibly Field-Induced Quantum Spin Liquid in $α − {RuCl}_{3}$
journal, November 2017

Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3
journal, November 2016

Linear spin wave theory for single-Q incommensurate magnetic structures
journal, March 2015

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

Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate
journal, June 2014

Unconventional spin dynamics in the honeycomb-lattice material $α − {RuCl}_{3}$ : High-field electron spin resonance studies
journal, December 2017

Effective model with strong Kitaev interactions for $α − {RuCl}_{3}$
journal, April 2018

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

Electronic and phonon excitations in $α - RuC l_{3}$
journal, October 2017

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

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

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

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

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

Hyperhoneycomb Iridate $β − {Li}_{2} {IrO}_{3}$ as a Platform for Kitaev Magnetism
journal, February 2015

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

Unusual Phonon Heat Transport in $α − {RuCl}_{3}$ : Strong Spin-Phonon Scattering and Field-Induced Spin Gap
journal, March 2018

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

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

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

Diagonalization of the quadratic boson hamiltonian
journal, September 1978

Relation between Kitaev magnetism and structure in $α - {RuCl}_{3}$
journal, May 2017

Anomalous Thermal Conductivity and Magnetic Torque Response in the Honeycomb Magnet $α − {RuCl}_{3}$
journal, May 2017

Fault-tolerant quantum computation by anyons
journal, January 2003

Emergent phenomena induced by spin–orbit coupling at surfaces and interfaces
journal, November 2016

Scanning X-ray microdiffraction with submicrometer white beam for strain/stress and orientation mapping in thin films
journal, February 2003

Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3
journal, December 2016

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

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3
journal, May 2015

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

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

Excitations in the field-induced quantum spin liquid state of α-RuCl3
text, January 2018

Generic spin model for the honeycomb iridates beyond the Kitaev limit
text, January 2013

Linear spin wave theory for single-Q incommensurate magnetic structures
text, January 2014

Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales
text, January 2016

Mechanism for subgap optical conductivity in honeycomb Kitaev materials
text, January 2017

Anyons in an exactly solved model and beyond
text, January 2005

Fault-tolerant quantum computation by anyons
text, January 1997

Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3
journal, January 2020

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

Kitaev honeycomb models in magnetic fields: Dynamical response and dual models
journal, October 2019

Two-step gap opening across the quantum critical point in the Kitaev honeycomb magnet $α − {RuCl}_{3}$
journal, January 2020

Two-step gap opening across the quantum critical point in a Kitaev honeycomb magnet
text, January 2018