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 00:00:00 EST 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 Laboratory (LANL), Los Alamos, NM (United States)

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

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1352414

Alternate ID(s):: OSTI ID: 1228795

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

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

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 329 works

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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
Probing and controlling magnetic states in 2D layered magnetic materials Mak, Kin Fai; Shan, Jie; Ralph, Daniel C. Nature Reviews Physics, Vol. 1, Issue 11 https://doi.org/10.1038/s42254-019-0110-y	journal	September 2019
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
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

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