Monoclinic crystal structure of α-RuCl3 and the zigzag antiferromagnetic ground state

Johnson, R. D.; Williams, S. C.; Haghighirad, A. A.; Singleton, J.; Zapf, V.; Manuel, P.; Mazin, I. I.; Li, Y.; Jeschke, H. O.; Valentí, R.; Coldea, R.

doi:10.1103/PhysRevB.92.235119

Title: Monoclinic crystal structure of $α - {RuCl}_{3}$ and the zigzag antiferromagnetic ground state

Journal Article · Thu Dec 10 04:00:00 UTC 2015 · Physical Review. B, Condensed Matter and Materials Physics

DOI: https://doi.org/10.1103/PhysRevB.92.235119 · OSTI ID:1352414

Johnson, R. D. ^[1]; Williams, S. C. ^[2]; Haghighirad, A. A. ^[2]; Singleton, J. ^[3]; Zapf, V. ^[3]; Manuel, P. ^[4]; Mazin, I. I. ^[5]; Li, Y. ^[6]; Jeschke, H. O. ^[6]; Valentí, R. ^[6]; Coldea, R. ^[2]

Univ. of Oxford (United Kingdom). Clarendon Lab.; Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Rutherford Appleton Lab., ISIS Neutron Source
Univ. of Oxford (United Kingdom). Clarendon Lab.
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). National High Magnetic Field Lab. (MagLab)
Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Rutherford Appleton Lab., ISIS Neutron Source
Naval Research Lab. (NRL), Washington, DC (United States)
Univ. of Frankfurt (Germany). Inst. for Theoretical Physics

We have proposed the layered honeycomb magnet α - RuCl ₃ as a candidate to realize a Kitaev spin model with strongly frustrated, bond-dependent, anisotropic interactions between spin-orbit entangled j _eff= 1/2 Ru ^{3 +} magnetic moments. We report a detailed study of the three-dimensional crystal structure using x-ray diffraction on untwinned crystals combined with structural relaxation calculations. We consider several models for the stacking of honeycomb layers and find evidence for a parent crystal structure with a monoclinic unit cell corresponding to a stacking of layers with a unidirectional in-plane offset, with occasional in-plane sliding stacking faults, in contrast with the currently assumed trigonal three-layer stacking periodicity. We also report electronic band-structure calculations for the monoclinic structure, which find support for the applicability of the j _eff = 1/2 picture once spin-orbit coupling and electron correlations are included. Of the three nearest-neighbor Ru-Ru bonds that comprise the honeycomb lattice, the monoclinic structure makes the bond parallel to the b axis nonequivalent to the other two, and we propose that the resulting differences in the magnitude of the anisotropic exchange along these bonds could provide a natural mechanism to explain the previously reported spin gap in powder inelastic neutron scattering measurements, in contrast to spin models based on the three-fold symmetric trigonal structure, which predict a gapless spectrum within linear spin wave theory. Our susceptibility measurements on both powders and stacked crystals, as well as magnetic neutron powder diffraction, show a single magnetic transition upon cooling below T _N ≈ 13 K. Our analysis of our neutron powder diffraction data provides evidence for zigzag magnetic order in the honeycomb layers with an antiferromagnetic stacking between layers. Magnetization measurements on stacked single crystals in pulsed field up to 60 T show a single transition around 8 T for in-plane fields followed by a gradual, asymptotic approach to magnetization saturation, as characteristic of strongly anisotropic exchange interactions.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1352414

Report Number(s):: LA-UR--15-27165

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Journal Name: Physical Review. B, Condensed Matter and Materials Physics Journal Issue: 23 Vol. 92; ISSN 1098-0121; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Relation between Kitaev magnetism and structure in α − RuCl 3 Glamazda, A.; Lemmens, P.; Do, S. -H. Physical Review B, Vol. 95, Issue 17 https://doi.org/10.1103/physrevb.95.174429	journal	May 2017
Phase diagram of α − RuCl 3 in an in-plane magnetic field Sears, J. A.; Zhao, Y.; Xu, Z. Physical Review B, Vol. 95, Issue 18 https://doi.org/10.1103/physrevb.95.180411	journal	May 2017
Resonant x-ray scattering reveals possible disappearance of magnetic order under hydrostatic pressure in the Kitaev candidate γ − Li 2 IrO 3 Breznay, Nicholas P.; Ruiz, Alejandro; Frano, Alex Physical Review B, Vol. 96, Issue 2 https://doi.org/10.1103/physrevb.96.020402	journal	July 2017
Majorana dynamical mean-field study of spin dynamics at finite temperatures in the honeycomb Kitaev model Yoshitake, Junki; Nasu, Joji; Kato, Yasuyuki Physical Review B, Vol. 96, Issue 2 https://doi.org/10.1103/physrevb.96.024438	journal	July 2017
Field-induced quantum criticality in the Kitaev system α − RuCl 3 Wolter, A. U. B.; Corredor, L. T.; Janssen, L. Physical Review B, Vol. 96, Issue 4 https://doi.org/10.1103/physrevb.96.041405	journal	July 2017
Magnetization processes of zigzag states on the honeycomb lattice: Identifying spin models for α − RuCl 3 and Na 2 IrO 3 Janssen, Lukas; Andrade, Eric C.; Vojta, Matthias Physical Review B, Vol. 96, Issue 6 https://doi.org/10.1103/physrevb.96.064430	journal	August 2017
Theoretical investigation of magnetic dynamics in α − RuCl 3 Wang, Wei; Dong, Zhao-Yang; Yu, Shun-Li Physical Review B, Vol. 96, Issue 11 https://doi.org/10.1103/physrevb.96.115103	journal	September 2017
Electronically highly cubic conditions for Ru in α − RuCl 3 Agrestini, S.; Kuo, C. -Y.; Ko, K. -T. Physical Review B, Vol. 96, Issue 16 https://doi.org/10.1103/physrevb.96.161107	journal	October 2017
Unconventional spin dynamics in the honeycomb-lattice material α − RuCl 3 : High-field electron spin resonance studies Ponomaryov, A. N.; Schulze, E.; Wosnitza, J. Physical Review B, Vol. 96, Issue 24 https://doi.org/10.1103/physrevb.96.241107	journal	December 2017
Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: α − Li 2 IrO 3 under pressure Hermann, V.; Altmeyer, M.; Ebad-Allah, J. Physical Review B, Vol. 97, Issue 2 https://doi.org/10.1103/physrevb.97.020104	journal	January 2018
Quantum spin liquid signatures in Kitaev-like frustrated magnets Gohlke, Matthias; Wachtel, Gideon; Yamaji, Youhei Physical Review B, Vol. 97, Issue 7 https://doi.org/10.1103/physrevb.97.075126	journal	February 2018
Role of spin-orbit coupling in the Kugel-Khomskii model on the honeycomb lattice Koga, Akihisa; Nakauchi, Shiryu; Nasu, Joji Physical Review B, Vol. 97, Issue 9 https://doi.org/10.1103/physrevb.97.094427	journal	March 2018
Magnetic structure and excitation spectrum of the hyperhoneycomb Kitaev magnet β − Li 2 IrO 3 Ducatman, Samuel; Rousochatzakis, Ioannis; Perkins, Natalia B. Physical Review B, Vol. 97, Issue 12 https://doi.org/10.1103/physrevb.97.125125	journal	March 2018
Effective model with strong Kitaev interactions for α − RuCl 3 Suzuki, Takafumi; Suga, Sei-ichiro Physical Review B, Vol. 97, Issue 13 https://doi.org/10.1103/physrevb.97.134424	journal	April 2018
Magnetic field induced evolution of intertwined orders in the Kitaev magnet β − Li 2 IrO 3 Rousochatzakis, Ioannis; Perkins, Natalia B. Physical Review B, Vol. 97, Issue 17 https://doi.org/10.1103/physrevb.97.174423	journal	May 2018
Dynamical and topological properties of the Kitaev model in a [111] magnetic field Gohlke, Matthias; Moessner, Roderich; Pollmann, Frank Physical Review B, Vol. 98, Issue 1 https://doi.org/10.1103/physrevb.98.014418	journal	July 2018
Classical and quantum spin dynamics of the honeycomb Γ model Samarakoon, Anjana M.; Wachtel, Gideon; Yamaji, Youhei Physical Review B, Vol. 98, Issue 4 https://doi.org/10.1103/physrevb.98.045121	journal	July 2018
Successive Majorana topological transitions driven by a magnetic field in the Kitaev model Nasu, Joji; Kato, Yasuyuki; Kamiya, Yoshitomo Physical Review B, Vol. 98, Issue 6 https://doi.org/10.1103/physrevb.98.060416	journal	August 2018
Field-induced magnon excitation and in-gap absorption in the Kitaev candidate RuCl 3 Shi, L. Y.; Liu, Y. Q.; Lin, T. Physical Review B, Vol. 98, Issue 9 https://doi.org/10.1103/physrevb.98.094414	journal	September 2018
Field evolution of magnons in α − RuCl 3 by high-resolution polarized terahertz spectroscopy Wu, Liang; Little, A.; Aldape, E. E. Physical Review B, Vol. 98, Issue 9 https://doi.org/10.1103/physrevb.98.094425	journal	September 2018
Ground-state phase diagram of the Kitaev-Heisenberg model on a kagome lattice Morita, Katsuhiro; Kishimoto, Masanori; Tohyama, Takami Physical Review B, Vol. 98, Issue 13 https://doi.org/10.1103/physrevb.98.134437	journal	October 2018
Signatures of low-energy fractionalized excitations in α − RuCl 3 from field-dependent microwave absorption Wellm, C.; Zeisner, J.; Alfonsov, A. Physical Review B, Vol. 98, Issue 18 https://doi.org/10.1103/physrevb.98.184408	journal	November 2018
Spin dynamics and field-induced magnetic phase transition in the honeycomb Kitaev magnet α − Li 2 IrO 3 Choi, Sungkyun; Manni, S.; Singleton, J. Physical Review B, Vol. 99, Issue 5 https://doi.org/10.1103/physrevb.99.054426	journal	February 2019
Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models Rusnačko, Juraj; Gotfryd, Dorota; Chaloupka, Jiří Physical Review B, Vol. 99, Issue 6 https://doi.org/10.1103/physrevb.99.064425	journal	February 2019
Magnetic anisotropy of the alkali iridate Na 2 IrO 3 at high magnetic fields: Evidence for strong ferromagnetic Kitaev correlations Das, Sitikantha D.; Kundu, Sarbajaya; Zhu, Zengwei Physical Review B, Vol. 99, Issue 8 https://doi.org/10.1103/physrevb.99.081101	journal	February 2019
Large thermal Hall effect in α − RuCl 3 : Evidence for heat transport by Kitaev-Heisenberg paramagnons Hentrich, Richard; Roslova, Maria; Isaeva, Anna Physical Review B, Vol. 99, Issue 8 https://doi.org/10.1103/physrevb.99.085136	journal	February 2019
Pressure-induced collapse of the spin-orbital Mott state in the hyperhoneycomb iridate β − Li 2 IrO 3 Takayama, T.; Krajewska, A.; Gibbs, A. S. Physical Review B, Vol. 99, Issue 12 https://doi.org/10.1103/physrevb.99.125127	journal	March 2019
Revisiting the Kitaev material candidacy of Ir 4 + double perovskite iridates Aczel, A. A.; Clancy, J. P.; Chen, Q. Physical Review B, Vol. 99, Issue 13 https://doi.org/10.1103/physrevb.99.134417	journal	April 2019
Observing spin fractionalization in the Kitaev spin liquid via temperature evolution of indirect resonant inelastic x-ray scattering Halász, Gábor B.; Kourtis, Stefanos; Knolle, Johannes Physical Review B, Vol. 99, Issue 18 https://doi.org/10.1103/physrevb.99.184417	journal	May 2019
Impact of off-diagonal exchange interactions on the Kitaev spin-liquid state of α − RuCl 3 Takikawa, Daichi; Fujimoto, Satoshi Physical Review B, Vol. 99, Issue 22 https://doi.org/10.1103/physrevb.99.224409	journal	June 2019
Ground state and low-energy excitations of the Kitaev-Heisenberg two-leg ladder Agrapidis, Cliò Efthimia; van den Brink, Jeroen; Nishimoto, Satoshi Physical Review B, Vol. 99, Issue 22 https://doi.org/10.1103/physrevb.99.224418	journal	June 2019
Hydrated lithium intercalation into the Kitaev spin liquid candidate material α − RuCl 3 Imai, Yoshinori; Konno, Katsuya; Hasegawa, Yoshinao Physical Review B, Vol. 99, Issue 24 https://doi.org/10.1103/physrevb.99.245141	journal	June 2019
J eff Description of the Honeycomb Mott Insulator α − RuCl 3 Koitzsch, A.; Habenicht, C.; Müller, E. Physical Review Letters, Vol. 117, Issue 12 https://doi.org/10.1103/physrevlett.117.126403	journal	September 2016
Resonant Inelastic X-Ray Scattering Response of the Kitaev Honeycomb Model Halász, Gábor B.; Perkins, Natalia B.; van den Brink, Jeroen Physical Review Letters, Vol. 117, Issue 12 https://doi.org/10.1103/physrevlett.117.127203	journal	September 2016
From a Quasimolecular Band Insulator to a Relativistic Mott Insulator in t 2 g 5 Systems with a Honeycomb Lattice Structure Kim, Beom Hyun; Shirakawa, Tomonori; Yunoki, Seiji Physical Review Letters, Vol. 117, Issue 18 https://doi.org/10.1103/physrevlett.117.187201	journal	October 2016
Spin-Wave Excitations Evidencing the Kitaev Interaction in Single Crystalline α − RuCl 3 Ran, Kejing; Wang, Jinghui; Wang, Wei Physical Review Letters, Vol. 118, Issue 10 https://doi.org/10.1103/physrevlett.118.107203	journal	March 2017
Classical Spin Liquid Instability Driven By Off-Diagonal Exchange in Strong Spin-Orbit Magnets Rousochatzakis, Ioannis; Perkins, Natalia B. Physical Review Letters, Vol. 118, Issue 14 https://doi.org/10.1103/physrevlett.118.147204	journal	April 2017
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
Probing α − RuCl 3 Beyond Magnetic Order: Effects of Temperature and Magnetic Field Winter, Stephen M.; Riedl, Kira; Kaib, David Physical Review Letters, Vol. 120, Issue 7 https://doi.org/10.1103/physrevlett.120.077203	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
Sawtooth Torque in Anisotropic j eff = 1 / 2 Magnets: Application to α − RuCl 3 Riedl, Kira; Li, Ying; Winter, Stephen M. Physical Review Letters, Vol. 122, Issue 19 https://doi.org/10.1103/physrevlett.122.197202	journal	May 2019
Giant Magnetic Anisotropy Induced by Ligand L S Coupling in Layered Cr Compounds Kim, Dong-Hwan; Kim, Kyoo; Ko, Kyung-Tae Physical Review Letters, Vol. 122, Issue 20 https://doi.org/10.1103/physrevlett.122.207201	journal	May 2019
Hidden Plaquette Order in a Classical Spin Liquid Stabilized by Strong Off-Diagonal Exchange Saha, Preetha; Fan, Zhijie; Zhang, Depei Physical Review Letters, Vol. 122, Issue 25 https://doi.org/10.1103/physrevlett.122.257204	journal	June 2019
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
Electronic Properties of α − RuCl 3 in Proximity to Graphene Biswas, Sananda; Li, Ying; Winter, Stephen M. Physical Review Letters, Vol. 123, Issue 23 https://doi.org/10.1103/physrevlett.123.237201	journal	December 2019
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
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
Collective spin dynamics of Z 2 vortex crystals in triangular Kitaev-Heisenberg antiferromagnets Li, Mengqun; Perkins, Natalia B.; Rousochatzakis, Ioannis Physical Review Research, Vol. 1, Issue 1 https://doi.org/10.1103/physrevresearch.1.013002	journal	August 2019
Magnetic field induced competing phases in spin-orbital entangled Kitaev magnets Chern, Li Ern; Kaneko, Ryui; Lee, Hyun-Yong Physical Review Research, Vol. 2, Issue 1 https://doi.org/10.1103/physrevresearch.2.013014	journal	January 2020
Unconventional magnetic field response of the hyperhoneycomb Kitaev magnet β − Li 2 IrO 3 Li, Mengqun; Rousochatzakis, Ioannis; Perkins, Natalia B. Physical Review Research, Vol. 2, Issue 1 https://doi.org/10.1103/physrevresearch.2.013065	journal	January 2020
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
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
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
Resonant inelastic X-ray scattering response of the Kitaev honeycomb model Halász, Gábor B.; Perkins, Natalia B.; Brink, Jeroen van den arXiv https://doi.org/10.48550/arxiv.1605.03272	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
Role of the spin-orbit coupling in the Kugel-Khomskii model on the honeycomb lattice Koga, Akihisa; Nakauchi, Shiryu; Nasu, Joji arXiv https://doi.org/10.48550/arxiv.1705.09659	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
Dynamical coupling of dilute magnetic impurities with quantum spin liquid state in the S = 3/2 dimer compound Ba3ZnRu2O9 Yamamoto, Takafumi D.; Taniguchi, Hiroki; Terasaki, Ichiro arXiv https://doi.org/10.48550/arxiv.1807.04076	text	January 2018
Observing spin fractionalization in the Kitaev spin liquid via temperature evolution of indirect resonant inelastic x-ray scattering Halász, Gábor B.; Kourtis, Stefanos; Knolle, Johannes arXiv https://doi.org/10.48550/arxiv.1811.04951	text	January 2018
Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models Rusnačko, Juraj; Gotfryd, Dorota; Chaloupka, Jiří arXiv https://doi.org/10.48550/arxiv.1902.07451	text	January 2019
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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Title: Monoclinic crystal structure of $α - {RuCl}_{3}$ and the zigzag antiferromagnetic ground state