Polarization-resolved Raman spectroscopy of α–RuCl3 and evidence of room-temperature two-dimensional magnetic scattering

Mai, Thuc T.; McCreary, Amber; Lampen-Kelley, Paige; Butch, N. P.; Simpson, J. R.; Yan, J. -Q.; Nagler, Stephen E.; Mandrus, David; Walker, A. R. Hight; Aguilar, Raul Valdés

doi:10.1103/PhysRevB.100.134419

Title: Polarization-resolved Raman spectroscopy of $α – {RuCl}_{3}$ and evidence of room-temperature two-dimensional magnetic scattering

Abstract

Polarization-resolved Raman spectroscopy was performed and analyzed from large, high-quality, monodomain single crystal of α–RuCl₃, a proximate Kitaev quantum spin liquid. Spectra were collected with laser polarizations parallel and perpendicular to the honeycomb plane. Pairs of nearly degenerate phonons were discovered and show either a fourfold or twofold polarization angle dependence in their Raman intensity, thereby providing evidence to definitively assign the bulk crystal point group as C_2h. The low-frequency continuum that is often attributed to scattering from pairs of Majorana fermions was also examined and found to disappear when the laser excitation and scattered photon polarizations were perpendicular to the honeycomb plane. This disappearance, along with the behavior of the phonon spectrum in the same polarization configuration, strongly suggests that the scattering continuum is two-dimensional. Here, we argue that this scattering continuum originates from the Kitaev magnetic interactions that survives up to room temperature, a scale larger than the bare Kitaev exchange energy of approximately 50 K.

Authors:

Mai, Thuc T. ^[1]; McCreary, Amber ^[2]; Lampen-Kelley, Paige ^[3]; Butch, N. P. ^[4]; Simpson, J. R. ^[5];

^[3];

^[6]; Mandrus, David ^[3]; Walker, A. R. Hight ^[2];

^[7]

The Ohio State Univ., Columbus, OH (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
Towson Univ., MD (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
The Ohio State Univ., Columbus, OH (United States)

Publication Date:: 2019-10-14

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); NSF MRSEC

OSTI Identifier:: 1606815

Grant/Contract Number:: AC05-00OR22725; DMR-1420451

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 100; Journal Issue: 13; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; magnetism; majorana fermions; phonons; quantum spin liquid; spin liquid; Raman spectroscopy

Citation Formats


                    Mai, Thuc T., McCreary, Amber, Lampen-Kelley, Paige, Butch, N. P., Simpson, J. R., Yan, J. -Q., Nagler, Stephen E., Mandrus, David, Walker, A. R. Hight, and Aguilar, Raul Valdés. Polarization-resolved Raman spectroscopy of α–RuCl3 and evidence of room-temperature two-dimensional magnetic scattering.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevB.100.134419.

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                    Mai, Thuc T., McCreary, Amber, Lampen-Kelley, Paige, Butch, N. P., Simpson, J. R., Yan, J. -Q., Nagler, Stephen E., Mandrus, David, Walker, A. R. Hight, & Aguilar, Raul Valdés. Polarization-resolved Raman spectroscopy of α–RuCl3 and evidence of room-temperature two-dimensional magnetic scattering.  United States.  https://doi.org/10.1103/PhysRevB.100.134419

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                    Mai, Thuc T., McCreary, Amber, Lampen-Kelley, Paige, Butch, N. P., Simpson, J. R., Yan, J. -Q., Nagler, Stephen E., Mandrus, David, Walker, A. R. Hight, and Aguilar, Raul Valdés. Mon .  
"Polarization-resolved Raman spectroscopy of α–RuCl3 and evidence of room-temperature two-dimensional magnetic scattering".  United States.  https://doi.org/10.1103/PhysRevB.100.134419.  https://www.osti.gov/servlets/purl/1606815.

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@article{osti_1606815,

  title        = {Polarization-resolved Raman spectroscopy of α–RuCl3 and evidence of room-temperature two-dimensional magnetic scattering},

  author       = {Mai, Thuc T. and McCreary, Amber and Lampen-Kelley, Paige and Butch, N. P. and Simpson, J. R. and Yan, J. -Q. and Nagler, Stephen E. and Mandrus, David and Walker, A. R. Hight and Aguilar, Raul Valdés},

  abstractNote = {Polarization-resolved Raman spectroscopy was performed and analyzed from large, high-quality, monodomain single crystal of α–RuCl3, a proximate Kitaev quantum spin liquid. Spectra were collected with laser polarizations parallel and perpendicular to the honeycomb plane. Pairs of nearly degenerate phonons were discovered and show either a fourfold or twofold polarization angle dependence in their Raman intensity, thereby providing evidence to definitively assign the bulk crystal point group as C2h. The low-frequency continuum that is often attributed to scattering from pairs of Majorana fermions was also examined and found to disappear when the laser excitation and scattered photon polarizations were perpendicular to the honeycomb plane. This disappearance, along with the behavior of the phonon spectrum in the same polarization configuration, strongly suggests that the scattering continuum is two-dimensional. Here, we argue that this scattering continuum originates from the Kitaev magnetic interactions that survives up to room temperature, a scale larger than the bare Kitaev exchange energy of approximately 50 K.},

  doi          = {10.1103/PhysRevB.100.134419},

  journal      = {Physical Review B},

  number       = 13,

  volume       = 100,

  place        = {United States},

  year         = {2019},

  month        = {10}

}

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https://doi.org/10.1103/PhysRevB.100.134419

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Cited by: 2 works

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Figures / Tables:

FIG. 1: Crystal structure and Laue X-ray diffraction pattern. Crystal structure of α-RuCl₃ projected onto the a-c plane (a) and a-b plane (b). The solid black lines represent the unit cell. The orange balls represent Cl atoms, while the larger blue balls represent Ru atoms. (c) Picture of studied sample;more »

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Works referenced in this record:

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Works referencing / citing this record:

Electronic Properties of $α − {RuCl}_{3}$ in Proximity to Graphene
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Similar Records

Title: Polarization-resolved Raman spectroscopy of α – RuCl 3 and evidence of room-temperature two-dimensional magnetic scattering

Abstract

Citation Formats

Figures / Tables:

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

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

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

Raman spectrum of CrI 3 : An ab initio study journal, August 2018

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

Theory of Raman response in three-dimensional Kitaev spin liquids: Application to β - and γ − Li 2 IrO 3 compounds journal, September 2015

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

Resonant Raman scattering theory for Kitaev models and their Majorana fermion boundary modes journal, September 2016

Fermionic response from fractionalization in an insulating two-dimensional magnet journal, July 2016

Electronic Structure of the Kitaev Material α-RuCl3 Probed by Photoemission and Inverse Photoemission Spectroscopies journal, December 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

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

Quantum spin liquids: a review journal, November 2016

Electrical Transport Signature of the Magnetic Fluctuation-Structure Relation in α-RuCl 3 Nanoflakes journal, April 2018

Lattice dynamics and phase transition in CrI 3 single crystals journal, September 2018

Lattice vibrations and Raman scattering in two-dimensional layered materials beyond graphene journal, September 2016

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

Sub-gap optical response in the Kitaev spin-liquid candidate α -RuCl 3 journal, November 2018

Effects of Configuration Interaction on Intensities and Phase Shifts journal, December 1961

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

Possible structural transformation and enhanced magnetic fluctuations in exfoliated α-RuCl3 journal, May 2019

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

A Field Guide to Spin Liquids journal, March 2019

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

Raman spectroscopic signature of fractionalized excitations in the harmonic-honeycomb iridates β- and γ-Li2IrO3 journal, July 2016

Quantum spin liquid at finite temperature: Proximate dynamics and persistent typicality journal, July 2019

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

Raman Scattering Signatures of Kitaev Spin Liquids in A 2 IrO 3 Iridates with A = Na or Li journal, October 2014

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

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

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

Raman spectroscopy evidence for dimerization and Mott collapse in α − RuCl 3 under pressures journal, February 2019

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

Physics of the Kitaev model: fractionalization, dynamical correlations, and material connections text, January 2018

Fermionic response from fractionalization in an insulating two-dimensional magnet text, January 2016

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

Resonant Raman scattering theory for Kitaev models and their Majorana fermion boundary modes text, January 2016

A Field Guide to Spin Liquids text, January 2018

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Title: Polarization-resolved Raman spectroscopy of $α – {RuCl}_{3}$ and evidence of room-temperature two-dimensional magnetic scattering

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

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

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

Raman spectrum of ${CrI}_{3}$ : An $ab initio$ study
journal, August 2018

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

Theory of Raman response in three-dimensional Kitaev spin liquids: Application to $β$ - and $γ - {Li}_{2} {IrO}_{3}$ compounds
journal, September 2015

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

Resonant Raman scattering theory for Kitaev models and their Majorana fermion boundary modes
journal, September 2016

Fermionic response from fractionalization in an insulating two-dimensional magnet
journal, July 2016

Electronic Structure of the Kitaev Material α-RuCl3 Probed by Photoemission and Inverse Photoemission Spectroscopies
journal, December 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

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

Quantum spin liquids: a review
journal, November 2016

Electrical Transport Signature of the Magnetic Fluctuation-Structure Relation in α-RuCl ₃ Nanoflakes
journal, April 2018

Lattice dynamics and phase transition in ${CrI}_{3}$ single crystals
journal, September 2018

Lattice vibrations and Raman scattering in two-dimensional layered materials beyond graphene
journal, September 2016

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

Sub-gap optical response in the Kitaev spin-liquid candidate α -RuCl ₃
journal, November 2018

Effects of Configuration Interaction on Intensities and Phase Shifts
journal, December 1961

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

Possible structural transformation and enhanced magnetic fluctuations in exfoliated α-RuCl3
journal, May 2019

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

A Field Guide to Spin Liquids
journal, March 2019

$α - {RuCl}_{3}$ : 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

Raman spectroscopic signature of fractionalized excitations in the harmonic-honeycomb iridates β- and γ-Li2IrO3
journal, July 2016

Quantum spin liquid at finite temperature: Proximate dynamics and persistent typicality
journal, July 2019

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

Raman Scattering Signatures of Kitaev Spin Liquids in $A_{2} {IrO}_{3}$ Iridates with $A = Na$ or Li
journal, October 2014

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

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

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

Raman spectroscopy evidence for dimerization and Mott collapse in $α − {RuCl}_{3}$ under pressures
journal, February 2019

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

Physics of the Kitaev model: fractionalization, dynamical correlations, and material connections
text, January 2018

Fermionic response from fractionalization in an insulating two-dimensional magnet
text, January 2016

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

Resonant Raman scattering theory for Kitaev models and their Majorana fermion boundary modes
text, January 2016

A Field Guide to Spin Liquids
text, January 2018

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

Electronic Properties of $α − {RuCl}_{3}$ in Proximity to Graphene
journal, December 2019

Field-induced ${QCD}_{3}$ -Chern-Simons quantum criticalities in Kitaev materials
journal, January 2020