Low-temperature crystal and magnetic structure of α – RuCl3

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.

doi:10.1103/PhysRevB.93.134423

Low-temperature crystal and magnetic structure of α – RuCl₃

Journal Article · Tue Apr 19 04:00:00 EDT 2016 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.93.134423· OSTI ID:1255683

Cao, Huibo B. ^[1]; Yan, Jiaqiang ^[2]; Bridges, Craig A. ^[1]; Lumsden, Mark D. ^[1]; Mandrus, D. G. ^[2]; Chakoumakos, Bryan C. ^[1]; Nagler, Stephen E. ^[2]; Banerjee, A. ^[1]; Tennant, D. A. ^[1]

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)

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 T_N = 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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1255683

Alternate ID(s):: OSTI ID: 1248067

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 13 Vol. 93; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Evidence for a Field-Induced Quantum Spin Liquid in α - RuCl 3 Baek, S. -H.; Do, S. -H.; Choi, K. -Y. Physical Review Letters, Vol. 119, Issue 3 https://doi.org/10.1103/physrevlett.119.037201	journal	July 2017
Antiferromagnetic Resonance and Terahertz Continuum in α − RuCl 3 Little, A.; Wu, Liang; Lampen-Kelley, P. Physical Review Letters, Vol. 119, Issue 22 https://doi.org/10.1103/physrevlett.119.227201	journal	November 2017
Magnetic Excitations and Continuum of a Possibly Field-Induced Quantum Spin Liquid in α − RuCl 3 Wang, Zhe; Reschke, S.; Hüvonen, D. Physical Review Letters, Vol. 119, Issue 22 https://doi.org/10.1103/physrevlett.119.227202	journal	November 2017
Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of α − RuCl 3 Zheng, Jiacheng; Ran, Kejing; Li, Tianrun Physical Review Letters, Vol. 119, Issue 22 https://doi.org/10.1103/physrevlett.119.227208	journal	December 2017
Ultralow-Temperature Thermal Conductivity of the Kitaev Honeycomb Magnet α − RuCl 3 across the Field-Induced Phase Transition Yu, Y. J.; Xu, Y.; Ran, K. J. Physical Review Letters, Vol. 120, Issue 6 https://doi.org/10.1103/physrevlett.120.067202	journal	February 2018
Unusual Phonon Heat Transport in α − RuCl 3 : Strong Spin-Phonon Scattering and Field-Induced Spin Gap Hentrich, Richard; Wolter, Anja U. B.; Zotos, Xenophon Physical Review Letters, Vol. 120, Issue 11 https://doi.org/10.1103/physrevlett.120.117204	journal	March 2018
Unusual Thermal Hall Effect in a Kitaev Spin Liquid Candidate α − RuCl 3 Kasahara, Y.; Sugii, K.; Ohnishi, T. Physical Review Letters, Vol. 120, Issue 21 https://doi.org/10.1103/physrevlett.120.217205	journal	May 2018
Microscopic Mechanism for a Higher-Spin Kitaev Model Stavropoulos, P. Peter; Pereira, D.; Kee, Hae-Young Physical Review Letters, Vol. 123, Issue 3 https://doi.org/10.1103/physrevlett.123.037203	journal	July 2019
One Proximate Kitaev Spin Liquid in the K − J − Γ Model on the Honeycomb Lattice Wang, Jiucai; Normand, B.; Liu, Zheng-Xin Physical Review Letters, Vol. 123, Issue 19 https://doi.org/10.1103/physrevlett.123.197201	journal	November 2019
Thermodynamic Evidence of Proximity to a Kitaev Spin Liquid in Ag 3 LiIr 2 O 6 Bahrami, Faranak; Lafargue-Dit-Hauret, William; Lebedev, Oleg I. Physical Review Letters, Vol. 123, Issue 23 https://doi.org/10.1103/physrevlett.123.237203	journal	December 2019
Magnetic behavior and spin-lattice coupling in cleavable van der Waals layered CrCl 3 crystals McGuire, Michael A.; Clark, Genevieve; Kc, Santosh Physical Review Materials, Vol. 1, Issue 1 https://doi.org/10.1103/physrevmaterials.1.014001	journal	June 2017
High-temperature magnetostructural transition in van der Waals-layered α − MoCl 3 McGuire, Michael A.; Yan, Jiaqiang; Lampen-Kelley, Paula Physical Review Materials, Vol. 1, Issue 6 https://doi.org/10.1103/physrevmaterials.1.064001	journal	November 2017
Magnetic ordering with an XY-like anisotropy in the honeycomb lattice iridates ZnIrO 3 and MgIrO 3 synthesized via a metathesis reaction Haraguchi, Yuya; Michioka, Chishiro; Matsuo, Akira Physical Review Materials, Vol. 2, Issue 5 https://doi.org/10.1103/physrevmaterials.2.054411	journal	May 2018
N i 2 M o 3 O 8 : Complex antiferromagnetic order on a honeycomb lattice Morey, Jennifer R.; Scheie, Allen; Sheckelton, John P. Physical Review Materials, Vol. 3, Issue 1 https://doi.org/10.1103/physrevmaterials.3.014410	journal	January 2019
Magnetic order in single crystals of Na 3 Co 2 SbO 6 with a honeycomb arrangement of 3 d 7 Co 2 + ions Yan, J. -Q.; Okamoto, S.; Wu, Y. Physical Review Materials, Vol. 3, Issue 7 https://doi.org/10.1103/physrevmaterials.3.074405	journal	July 2019
Crystal structure and magnetic properties of the layered van der Waals compound VB r 3 Kong, Tai; Guo, Shu; Ni, Danrui Physical Review Materials, Vol. 3, Issue 8 https://doi.org/10.1103/physrevmaterials.3.084419	journal	August 2019
Synthesis, magnetization, and heat capacity of triangular lattice materials NaErSe 2 and KErSe 2 Xing, Jie; Sanjeewa, Liurukara D.; Kim, Jungsoo Physical Review Materials, Vol. 3, Issue 11 https://doi.org/10.1103/physrevmaterials.3.114413	journal	November 2019
Field-induced QCD 3 -Chern-Simons quantum criticalities in Kitaev materials Zou, Liujun; He, Yin-Chen Physical Review Research, Vol. 2, Issue 1 https://doi.org/10.1103/physrevresearch.2.013072	journal	January 2020
Approximately Quantized Thermal Hall Effect of Chiral Liquids Coupled to Phonons Vinkler-Aviv, Yuval; Rosch, Achim Physical Review X, Vol. 8, Issue 3 https://doi.org/10.1103/physrevx.8.031032	journal	August 2018
Weak-field induced nonmagnetic state in a Co-based honeycomb Zhong, Ruidan; Gao, Tong; Ong, Nai Phuan Science Advances, Vol. 6, Issue 4 https://doi.org/10.1126/sciadv.aay6953	journal	January 2020
Neutron scattering in the proximate quantum spin liquid α-RuCl ₃ Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes Science, Vol. 356, Issue 6342 https://doi.org/10.1126/science.aah6015	journal	June 2017
Quantum spin liquids Broholm, C.; Cava, R. J.; Kivelson, S. A. Science, Vol. 367, Issue 6475 https://doi.org/10.1126/science.aay0668	journal	January 2020
Neutron scattering in the proximate quantum spin liquid α-RuCl3. Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.11028	text	January 2017
Excitations in the field-induced quantum spin liquid state of α-RuCl3 Banerjee, A.; Lampen-Kelley, P.; Knolle, Johannes Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.11029	text	January 2018
Magnetic anisotropy of the alkali iridate Na2IrO3 at high magnetic fields: Evidence for strong ferromagnetic Kitaev correlations Das, Sd; Kundu, S.; Zhu, Z. Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.37427	text	January 2019
Pressure-Tuned Interactions in Frustrated Magnets: Pathway to Quantum Spin Liquids? Biesner, Tobias; Uykur, Ece Crystals, Vol. 10, Issue 1 https://doi.org/10.3390/cryst10010004	journal	December 2019
Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides McGuire, Michael Crystals, Vol. 7, Issue 5 https://doi.org/10.3390/cryst7050121	journal	April 2017
Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales Winter, Stephen M.; Li, Ying; Jeschke, Harald O. arXiv https://doi.org/10.48550/arxiv.1603.02548	text	January 2016
Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides McGuire, Michael A. arXiv https://doi.org/10.48550/arxiv.1704.08225	text	January 2017
Uniaxial and hydrostatic pressure effects in alpha-RuCl3 single crystals via thermal-expansion measurements He, Mingquan; Wang, Xiao; Wang, Liran arXiv https://doi.org/10.48550/arxiv.1712.08511	text	January 2017
Interlayer Coupling Effect on a Bilayer Kitaev Model Tomishige, Hiroyuki; Nasu, Joji; Koga, Akihisa arXiv https://doi.org/10.48550/arxiv.1712.09050	text	January 2017
Two-step gap opening across the quantum critical point in a Kitaev honeycomb magnet Nagai, Y.; Jinno, T.; Yoshitake, Y. arXiv https://doi.org/10.48550/arxiv.1810.05379	text	January 2018
Microscopic mechanism for higher-spin Kitaev model Stavropoulos, P. Peter; Pereira, D.; Kee, Hae-Young arXiv https://doi.org/10.48550/arxiv.1903.00011	text	January 2019
Observation of two types of fractional excitation in the Kitaev honeycomb magnet Jansa, N.; Zorko, A.; Gomilsek, M. Nature Publishing Group https://doi.org/10.7892/boris.118887	text	January 2018

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