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 »
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- 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}
}
Web of Science
Works referenced in this record:
Anyons in an exactly solved model and beyond
journal, January 2006
- Kitaev, Alexei
- Annals of Physics, Vol. 321, Issue 1
Non-Abelian anyons and topological quantum computation
journal, September 2008
- Nayak, Chetan; Simon, Steven H.; Stern, Ady
- Reviews of Modern Physics, Vol. 80, Issue 3
Highly Mobile Gapless Excitations in a Two-Dimensional Candidate Quantum Spin Liquid
journal, June 2010
- Yamashita, M.; Nakata, N.; Senshu, Y.
- Science, Vol. 328, Issue 5983
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
Dynamics of a Two-Dimensional Quantum Spin Liquid: Signatures of Emergent Majorana Fermions and Fluxes
journal, May 2014
- Knolle, J.; Kovrizhin, D. L.; Chalker, J. T.
- Physical Review Letters, Vol. 112, Issue 20
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009
- Jackeli, G.; Khaliullin, G.
- Physical Review Letters, Vol. 102, Issue 1
Antiferromagnetic Mott insulating state in single crystals of the honeycomb lattice material
journal, August 2010
- Singh, Yogesh; Gegenwart, P.
- Physical Review B, Vol. 82, Issue 6
Unconventional magnetic order on the hyperhoneycomb Kitaev lattice in : Full solution via magnetic resonant x-ray diffraction
journal, November 2014
- Biffin, A.; Johnson, R. D.; Choi, Sungkyun
- Physical Review B, Vol. 90, Issue 20
Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
journal, March 2016
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- Annual Review of Condensed Matter Physics, Vol. 7, Issue 1
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
Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates
journal, March 2012
- Singh, Yogesh; Manni, S.; Reuther, J.
- Physical Review Letters, Vol. 108, Issue 12
Zigzag Magnetic Order in the Iridium Oxide
journal, February 2013
- Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat
- Physical Review Letters, Vol. 110, Issue 9
Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in
journal, November 2014
- Biffin, A.; Johnson, R. D.; Kimchi, I.
- Physical Review Letters, Vol. 113, Issue 19
Spin Waves and Revised Crystal Structure of Honeycomb Iridate
journal, March 2012
- Choi, S. K.; Coldea, R.; Kolmogorov, A. N.
- Physical Review Letters, Vol. 108, Issue 12
Direct evidence of a zigzag spin-chain structure in the honeycomb lattice: A neutron and x-ray diffraction investigation of single-crystal Na IrO
journal, May 2012
- Ye, Feng; Chi, Songxue; Cao, Huibo
- Physical Review B, Vol. 85, Issue 18
Magnetic order in : A honeycomb-lattice quantum magnet with strong spin-orbit coupling
journal, April 2015
- Sears, J. A.; Songvilay, M.; Plumb, K. W.
- Physical Review B, Vol. 91, Issue 14
Scattering Continuum and Possible Fractionalized Excitations in
journal, April 2015
- Sandilands, Luke J.; Tian, Yao; Plumb, Kemp W.
- Physical Review Letters, Vol. 114, Issue 14
Anisotropic magnetism in the honeycomb system: Susceptibility, specific heat, and zero-field NMR
journal, May 2015
- Majumder, M.; Schmidt, M.; Rosner, H.
- Physical Review B, Vol. 91, Issue 18
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
Monoclinic crystal structure of and the zigzag antiferromagnetic ground state
journal, December 2015
- Johnson, R. D.; Williams, S. C.; Haghighirad, A. A.
- Physical Review B, Vol. 92, Issue 23
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
Successive magnetic phase transitions in : XY-like frustrated magnet on the honeycomb lattice
journal, March 2015
- Kubota, Yumi; Tanaka, Hidekazu; Ono, Toshio
- Physical Review B, Vol. 91, Issue 9
Anhydrous Ruthenium Chlorides
journal, September 1963
- Fletcher, J. M.; Gardner, W. E.; Hooper, E. W.
- Nature, Vol. 199, Issue 4898
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
Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides
journal, July 2010
- Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat
- Physical Review Letters, Vol. 105, Issue 2
Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit
journal, February 2014
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- Physical Review Letters, Vol. 112, Issue 7
Hidden symmetries of the extended Kitaev-Heisenberg model: Implications for the honeycomb-lattice iridates
journal, July 2015
- Chaloupka, Jiří; Khaliullin, Giniyat
- Physical Review B, Vol. 92, Issue 2
Phase Diagram and Quantum Order by Disorder in the Kitaev Honeycomb Magnet
journal, December 2015
- Rousochatzakis, Ioannis; Reuther, Johannes; Thomale, Ronny
- Physical Review X, Vol. 5, Issue 4
Experimental and theoretical studies of the mica polymorphs
journal, September 1956
- Smith, J. V.; Yoder, H. S.
- Mineralogical Magazine and Journal of the Mineralogical Society, Vol. 31, Issue 234
Die struktur des IrBr3 und über die ursachen der fehlordnungserscheinungen bei den in schichtenstrukturen kristallisierenden edelmetalltrihalogeniden
journal, July 1968
- Brodersen, K.; Thiele, G.; Ohnsorge, H.
- Journal of the Less Common Metals, Vol. 15, Issue 3
α- and β-ruthenium trichloride
journal, June 1965
- Hyde, K. R.; Hooper, E. W.; Waters, J.
- Journal of the Less Common Metals, Vol. 8, Issue 6
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
WinGX and ORTEP for Windows : an update
journal, July 2012
- Farrugia, Louis J.
- Journal of Applied Crystallography, Vol. 45, Issue 4
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
VESTA : a three-dimensional visualization system for electronic and structural analysis
journal, May 2008
- Momma, Koichi; Izumi, Fujio
- Journal of Applied Crystallography, Vol. 41, Issue 3
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
Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993
- Rodríguez-Carvajal, Juan
- Physica B: Condensed Matter, Vol. 192, Issue 1-2
The Lattice Vibration Specific Heat of Graphite
journal, October 1953
- Krumhansl, J.; Brooks, H.
- The Journal of Chemical Physics, Vol. 21, Issue 10
Cation Ordering in Layered O3 Li[Ni x Li 1/3 - 2 x /3 Mn 2/ 3 - x /3 ]O 2 (0 ≤ x ≤ 1 / 2 ) Compounds
journal, May 2005
- Meng, Y. S.; Ceder, G.; Grey, C. P.
- Chemistry of Materials, Vol. 17, Issue 9
Orbital Order and Fluctuations in Mott Insulators
journal, January 2005
- Khaliullin, Giniyat
- Progress of Theoretical Physics Supplement, Vol. 160
Non-Abelian Anyons and Topological Quantum Computation
text, January 2007
- Nayak, Chetan; Simon, Steven H.; Stern, Ady
- arXiv
Generic spin model for the honeycomb iridates beyond the Kitaev limit
text, January 2013
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- arXiv
Works referencing / citing this record:
Resonant torsion magnetometry in anisotropic quantum materials
journal, September 2018
- Modic, K. A.; Bachmann, Maja D.; Ramshaw, B. J.
- Nature Communications, Vol. 9, Issue 1
Theory of the field-revealed Kitaev spin liquid
journal, June 2019
- Gordon, Jacob S.; Catuneanu, Andrei; Sørensen, Erik S.
- Nature Communications, Vol. 10, Issue 1
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
Path to stable quantum spin liquids in spin-orbit coupled correlated materials
journal, April 2018
- Catuneanu, Andrei; Yamaji, Youhei; Wachtel, Gideon
- npj Quantum Materials, Vol. 3, Issue 1
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
Switching 2D magnetic states via pressure tuning of layer stacking
journal, October 2019
- Song, Tiancheng; Fei, Zaiyao; Yankowitz, Matthew
- Nature Materials, Vol. 18, Issue 12
Pressure-controlled interlayer magnetism in atomically thin CrI3
journal, October 2019
- Li, Tingxin; Jiang, Shengwei; Sivadas, Nikhil
- Nature Materials, Vol. 18, Issue 12
Enhancement of interlayer exchange in an ultrathin two-dimensional magnet
journal, September 2019
- Klein, Dahlia R.; MacNeill, David; Song, Qian
- Nature Physics, Vol. 15, Issue 12
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
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
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
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
Two-step gap opening across the quantum critical point in the Kitaev honeycomb magnet
journal, January 2020
- Nagai, Yuya; Jinno, Takaaki; Yoshitake, Junki
- Physical Review B, Vol. 101, Issue 2
Selection of direction of the ordered moments in and
journal, August 2016
- Sizyuk, Yuriy; Wölfle, Peter; Perkins, Natalia B.
- Physical Review B, Vol. 94, Issue 8
Interlayer coupling effect on a bilayer Kitaev model
journal, March 2018
- Tomishige, Hiroyuki; Nasu, Joji; Koga, Akihisa
- Physical Review B, Vol. 97, Issue 9
Field evolution of magnons in by high-resolution polarized terahertz spectroscopy
journal, September 2018
- Wu, Liang; Little, A.; Aldape, E. E.
- Physical Review B, Vol. 98, Issue 9
Chiral spin order in some purported Kitaev spin-liquid compounds
journal, November 2018
- Modic, K. A.; Ramshaw, B. J.; Shekhter, A.
- Physical Review B, Vol. 98, Issue 20
Magnetic anisotropy of the alkali iridate at high magnetic fields: Evidence for strong ferromagnetic Kitaev correlations
journal, February 2019
- Das, Sitikantha D.; Kundu, Sarbajaya; Zhu, Zengwei
- Physical Review B, Vol. 99, Issue 8
Hydrated lithium intercalation into the Kitaev spin liquid candidate material α − RuCl 3
journal, June 2019
- Imai, Yoshinori; Konno, Katsuya; Hasegawa, Yoshinao
- Physical Review B, Vol. 99, Issue 24
Magnetic ordering with an XY-like anisotropy in the honeycomb lattice iridates and synthesized via a metathesis reaction
journal, May 2018
- Haraguchi, Yuya; Michioka, Chishiro; Matsuo, Akira
- Physical Review Materials, Vol. 2, Issue 5
Field-induced -Chern-Simons quantum criticalities in Kitaev materials
journal, January 2020
- Zou, Liujun; He, Yin-Chen
- Physical Review Research, Vol. 2, Issue 1
Weak-field induced nonmagnetic state in a Co-based honeycomb
journal, January 2020
- Zhong, Ruidan; Gao, Tong; Ong, Nai Phuan
- Science Advances, Vol. 6, Issue 4
Neutron scattering in the proximate quantum spin liquid α-RuCl 3
journal, June 2017
- Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes
- Science, Vol. 356, Issue 6342
Quantum spin liquids
journal, January 2020
- Broholm, C.; Cava, R. J.; Kivelson, S. A.
- Science, Vol. 367, Issue 6475
Pressure-Tuned Interactions in Frustrated Magnets: Pathway to Quantum Spin Liquids?
journal, December 2019
- Biesner, Tobias; Uykur, Ece
- Crystals, Vol. 10, Issue 1
Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides
journal, April 2017
- McGuire, Michael
- Crystals, Vol. 7, Issue 5
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
Concept and realization of Kitaev quantum spin liquids
journal, March 2019
- Takagi, Hidenori; Takayama, Tomohiro; Jackeli, George
- Nature Reviews Physics, Vol. 1, Issue 4
2D proximate quantum spin liquid state in atomic-thin α -RuCl 3
journal, November 2018
- Du, Luojun; Huang, Yuan; Wang, Yimeng
- 2D Materials, Vol. 6, Issue 1
Observation of two types of fractional excitation in the Kitaev honeycomb magnet
text, January 2018
- Jansa, N.; Zorko, A.; Gomilsek, M.
- Nature Publishing Group
Observation of two types of fractional excitation in the Kitaev honeycomb magnet
journal, May 2018
- Janša, Nejc; Zorko, Andrej; Gomilšek, Matjaž
- Nature Physics, Vol. 14, Issue 8
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
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
Neutron scattering in the proximate quantum spin liquid α-RuCl3.
text, January 2017
- Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes
- Apollo - University of Cambridge Repository
Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales
text, January 2016
- Winter, Stephen M.; Li, Ying; Jeschke, Harald O.
- arXiv
Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides
text, January 2017
- McGuire, Michael A.
- arXiv
Uniaxial and hydrostatic pressure effects in alpha-RuCl3 single crystals via thermal-expansion measurements
text, January 2017
- He, Mingquan; Wang, Xiao; Wang, Liran
- arXiv
Interlayer Coupling Effect on a Bilayer Kitaev Model
text, January 2017
- Tomishige, Hiroyuki; Nasu, Joji; Koga, Akihisa
- arXiv
Two-step gap opening across the quantum critical point in a Kitaev honeycomb magnet
text, January 2018
- Nagai, Y.; Jinno, T.; Yoshitake, Y.
- arXiv
Microscopic mechanism for higher-spin Kitaev model
text, January 2019
- Stavropoulos, P. Peter; Pereira, D.; Kee, Hae-Young
- arXiv