DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Low-temperature crystal and magnetic structure of α – RuCl3

Abstract

Here, single crystals of the Kitaev spin-liquid candidate α – RuCl3 have been studied to determine the low-temperature bulk properties, the structure, and the magnetic ground state. Refinements of x-ray diffraction data show that the low-temperature crystal structure is described by space group C2/m with a nearly perfect honeycomb lattice exhibiting less than 0.2% in-plane distortion. The as-grown single crystals exhibit only one sharp magnetic transition at TN = 7 K. The magnetic order below this temperature exhibits a propagation vector of k=(0,1,1/3), which coincides with a three-layer stacking of the C2/m unit cells. Magnetic transitions at higher temperatures up to 14 K can be introduced by deformations of the crystal that result in regions in the crystal with a two-layer stacking sequence. The best-fit symmetry-allowed magnetic structure of the as-grown crystals shows that the spins lie in the ac plane, with a zigzag configuration in each honeycomb layer. The three-layer repeat out-of-plane structure can be refined as a 120° spiral order or a collinear structure with a spin direction of 35° away from the a axis. The collinear spin configuration yields a slightly better fit and also is physically preferred. The average ordered moment in either structure is lessmore » than 0.45(5) μB per Ru3+ ion.« less

Authors:
 [1];  [2];  [1];  [1];  [2];  [1];  [2];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1255683
Alternate Identifier(s):
OSTI ID: 1248067
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 93; 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

Citation Formats

Cao, Huibo B., Yan, Jiaqiang, Bridges, Craig A., Lumsden, Mark D., Mandrus, D. G., Chakoumakos, Bryan C., Nagler, Stephen E., Banerjee, A., and Tennant, D. A. Low-temperature crystal and magnetic structure of α – RuCl3. United States: N. p., 2016. Web. doi:10.1103/PhysRevB.93.134423.
Cao, Huibo B., Yan, Jiaqiang, Bridges, Craig A., Lumsden, Mark D., Mandrus, D. G., Chakoumakos, Bryan C., Nagler, Stephen E., Banerjee, A., & Tennant, D. A. Low-temperature crystal and magnetic structure of α – RuCl3. United States. https://doi.org/10.1103/PhysRevB.93.134423
Cao, Huibo B., Yan, Jiaqiang, Bridges, Craig A., Lumsden, Mark D., Mandrus, D. G., Chakoumakos, Bryan C., Nagler, Stephen E., Banerjee, A., and Tennant, D. A. Tue . "Low-temperature crystal and magnetic structure of α – RuCl3". United States. https://doi.org/10.1103/PhysRevB.93.134423. https://www.osti.gov/servlets/purl/1255683.
@article{osti_1255683,
title = {Low-temperature crystal and magnetic structure of α – RuCl3},
author = {Cao, Huibo B. and Yan, Jiaqiang and Bridges, Craig A. and Lumsden, Mark D. and Mandrus, D. G. and Chakoumakos, Bryan C. and Nagler, Stephen E. and Banerjee, A. and Tennant, D. A.},
abstractNote = {Here, single crystals of the Kitaev spin-liquid candidate α – RuCl3 have been studied to determine the low-temperature bulk properties, the structure, and the magnetic ground state. Refinements of x-ray diffraction data show that the low-temperature crystal structure is described by space group C2/m with a nearly perfect honeycomb lattice exhibiting less than 0.2% in-plane distortion. The as-grown single crystals exhibit only one sharp magnetic transition at TN = 7 K. The magnetic order below this temperature exhibits a propagation vector of k=(0,1,1/3), which coincides with a three-layer stacking of the C2/m unit cells. Magnetic transitions at higher temperatures up to 14 K can be introduced by deformations of the crystal that result in regions in the crystal with a two-layer stacking sequence. The best-fit symmetry-allowed magnetic structure of the as-grown crystals shows that the spins lie in the ac plane, with a zigzag configuration in each honeycomb layer. The three-layer repeat out-of-plane structure can be refined as a 120° spiral order or a collinear structure with a spin direction of 35° away from the a axis. The collinear spin configuration yields a slightly better fit and also is physically preferred. The average ordered moment in either structure is less than 0.45(5) μB per Ru3+ ion.},
doi = {10.1103/PhysRevB.93.134423},
journal = {Physical Review B},
number = 13,
volume = 93,
place = {United States},
year = {Tue Apr 19 00:00:00 EDT 2016},
month = {Tue Apr 19 00:00:00 EDT 2016}
}

Journal Article:

Citation Metrics:
Cited by: 226 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

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


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


Highly Mobile Gapless Excitations in a Two-Dimensional Candidate Quantum Spin Liquid
journal, June 2010


Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet
journal, December 2012

  • Han, Tian-Heng; Helton, Joel S.; Chu, Shaoyan
  • Nature, Vol. 492, Issue 7429
  • DOI: 10.1038/nature11659

Dynamics of a Two-Dimensional Quantum Spin Liquid: Signatures of Emergent Majorana Fermions and Fluxes
journal, May 2014


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


Antiferromagnetic Mott insulating state in single crystals of the honeycomb lattice material Na 2 IrO 3
journal, August 2010


Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
journal, March 2016


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

  • Hwan Chun, Sae; Kim, Jong-Woo; Kim, Jungho
  • Nature Physics, Vol. 11, Issue 6
  • DOI: 10.1038/nphys3322

Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates A 2 IrO 3
journal, March 2012


Zigzag Magnetic Order in the Iridium Oxide Na 2 IrO 3
journal, February 2013


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


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


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


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


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


Moessbauer spectroscopy and magnetization studies of .alpha.- and .beta.-ruthenium trichloride
journal, October 1992

  • Kobayashi, Y.; Okada, T.; Asai, K.
  • Inorganic Chemistry, Vol. 31, Issue 22
  • DOI: 10.1021/ic00048a025

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


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

  • Banerjee, A.; Bridges, C. A.; Yan, J. -Q.
  • Nature Materials, Vol. 15, Issue 7
  • DOI: 10.1038/nmat4604

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


Anhydrous Ruthenium Chlorides
journal, September 1963

  • Fletcher, J. M.; Gardner, W. E.; Hooper, E. W.
  • Nature, Vol. 199, Issue 4898
  • DOI: 10.1038/1991089a0

X-Ray, infrared, and magnetic studies of α- and β-ruthenium trichloride
journal, January 1967

  • Fletcher, J. M.; Gardner, W. E.; Fox, A. C.
  • J. Chem. Soc. A, Vol. 0, Issue 0
  • DOI: 10.1039/J19670001038

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


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


Hidden symmetries of the extended Kitaev-Heisenberg model: Implications for the honeycomb-lattice iridates A 2 IrO 3
journal, July 2015


Phase Diagram and Quantum Order by Disorder in the Kitaev K 1 K 2 Honeycomb Magnet
journal, December 2015

  • Rousochatzakis, Ioannis; Reuther, Johannes; Thomale, Ronny
  • Physical Review X, Vol. 5, Issue 4
  • DOI: 10.1103/PhysRevX.5.041035

Experimental and theoretical studies of the mica polymorphs
journal, September 1956


Die struktur des IrBr3 und über die ursachen der fehlordnungserscheinungen bei den in schichtenstrukturen kristallisierenden edelmetalltrihalogeniden
journal, July 1968


α- and β-ruthenium trichloride
journal, June 1965


A short history of SHELX
journal, December 2007

  • Sheldrick, George M.
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 64, Issue 1, p. 112-122
  • DOI: 10.1107/S0108767307043930

WinGX and ORTEP for Windows : an update
journal, July 2012


Automated determination of the extinction symbol via electron diffraction data
journal, March 2012

  • Camalli, Mercedes; Carrozzini, Benedetta; Cascarano, Giovanni Luca
  • Journal of Applied Crystallography, Vol. 45, Issue 2
  • DOI: 10.1107/S0021889812003317

VESTA : a three-dimensional visualization system for electronic and structural analysis
journal, May 2008


Four-circle single-crystal neutron diffractometer at the High Flux Isotope Reactor
journal, May 2011

  • Chakoumakos, Bryan C.; Cao, Huibo; Ye, Feng
  • Journal of Applied Crystallography, Vol. 44, Issue 3
  • DOI: 10.1107/S0021889811012301

Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993


The Lattice Vibration Specific Heat of Graphite
journal, October 1953

  • Krumhansl, J.; Brooks, H.
  • The Journal of Chemical Physics, Vol. 21, Issue 10
  • DOI: 10.1063/1.1698641

Cation Ordering in Layered O3 Li[Ni x Li 1/3 - 2 x /3 Mn 2/ 3 - x /3 ]O 2 (0 ≤ x1 / 2 ) Compounds
journal, May 2005

  • Meng, Y. S.; Ceder, G.; Grey, C. P.
  • Chemistry of Materials, Vol. 17, Issue 9
  • DOI: 10.1021/cm047779m

Orbital Order and Fluctuations in Mott Insulators
journal, January 2005

  • Khaliullin, Giniyat
  • Progress of Theoretical Physics Supplement, Vol. 160
  • DOI: 10.1143/PTPS.160.155

Non-Abelian Anyons and Topological Quantum Computation
text, January 2007


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


Works referencing / citing this record:

Resonant torsion magnetometry in anisotropic quantum materials
journal, September 2018


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


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

  • Banerjee, Arnab; Lampen-Kelley, Paula; Knolle, Johannes
  • npj Quantum Materials, Vol. 3, Issue 1
  • DOI: 10.1038/s41535-018-0079-2

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


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


Switching 2D magnetic states via pressure tuning of layer stacking
journal, October 2019


Pressure-controlled interlayer magnetism in atomically thin CrI3
journal, October 2019


Enhancement of interlayer exchange in an ultrathin two-dimensional magnet
journal, September 2019


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

  • Yadav, Ravi; Bogdanov, Nikolay A.; Katukuri, Vamshi M.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep37925

Electronic Structure of the Kitaev Material α-RuCl3 Probed by Photoemission and Inverse Photoemission Spectroscopies
journal, December 2016

  • Sinn, Soobin; Kim, Choong Hyun; Kim, Beom Hyun
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep39544

Strain effects on electronic and magnetic properties of the monolayer α - RuCl 3: A first-principles and Monte Carlo study
journal, February 2019

  • Vatansever, Erol; Sarikurt, Sevil; Ersan, Fatih
  • Journal of Applied Physics, Vol. 125, Issue 8
  • DOI: 10.1063/1.5078713

Quasi-degenerate magnetic states in α-RuCl 3
journal, December 2018

  • Yang, Huan-Cheng; Gong, Ben-Chao; Liu, Kai
  • Journal of Physics: Condensed Matter, Vol. 31, Issue 2
  • DOI: 10.1088/1361-648x/aaeeac

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


Selection of direction of the ordered moments in Na 2 IrO 3 and α RuCl 3
journal, August 2016


Interlayer coupling effect on a bilayer Kitaev model
journal, March 2018


Field evolution of magnons in α RuCl 3 by high-resolution polarized terahertz spectroscopy
journal, September 2018


Chiral spin order in some purported Kitaev spin-liquid compounds
journal, November 2018


Magnetic anisotropy of the alkali iridate Na 2 IrO 3 at high magnetic fields: Evidence for strong ferromagnetic Kitaev correlations
journal, February 2019


Hydrated lithium intercalation into the Kitaev spin liquid candidate material α − RuCl 3
journal, June 2019


Magnetic ordering with an XY-like anisotropy in the honeycomb lattice iridates ZnIrO 3 and MgIrO 3 synthesized via a metathesis reaction
journal, May 2018


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


Weak-field induced nonmagnetic state in a Co-based honeycomb
journal, January 2020


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


Quantum spin liquids
journal, January 2020


Pressure-Tuned Interactions in Frustrated Magnets: Pathway to Quantum Spin Liquids?
journal, December 2019


Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides
journal, April 2017


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

  • Do, Seung-Hwan; Park, Sang-Youn; Yoshitake, Junki
  • Nature Physics, Vol. 13, Issue 11
  • DOI: 10.1038/nphys4264

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

  • Takagi, Hidenori; Takayama, Tomohiro; Jackeli, George
  • Nature Reviews Physics, Vol. 1, Issue 4
  • DOI: 10.1038/s42254-019-0038-2

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


Observation of two types of fractional excitation in the Kitaev honeycomb magnet
text, January 2018


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


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

  • Banerjee, A.; Lampen-Kelley, P.; Knolle, Johannes
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.11029

Magnetic anisotropy of the alkali iridate Na2IrO3 at high magnetic fields: Evidence for strong ferromagnetic Kitaev correlations
text, January 2019

  • Das, Sd; Kundu, S.; Zhu, Z.
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.37427

Neutron scattering in the proximate quantum spin liquid α-RuCl3.
text, January 2017

  • Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.11028

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


Interlayer Coupling Effect on a Bilayer Kitaev Model
text, January 2017


Microscopic mechanism for higher-spin Kitaev model
text, January 2019