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Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet

Nature Materials volume 15, pages 733–740 (2016)Cite this article

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Abstract

Quantum spin liquids (QSLs) are topological states of matter exhibiting remarkable properties such as the capacity to protect quantum information from decoherence. Whereas their featureless ground states have precluded their straightforward experimental identification, excited states are more revealing and particularly interesting owing to the emergence of fundamentally new excitations such as Majorana fermions. Ideal probes of these excitations are inelastic neutron scattering experiments. These we report here for a ruthenium-based material, α-RuCl3, continuing a major search (so far concentrated on iridium materials) for realizations of the celebrated Kitaev honeycomb topological QSL. Our measurements confirm the requisite strong spin–orbit coupling and low-temperature magnetic order matching predictions proximate to the QSL. We find stacking faults, inherent to the highly two-dimensional nature of the material, resolve an outstanding puzzle. Crucially, dynamical response measurements above interlayer energy scales are naturally accounted for in terms of deconfinement physics expected for QSLs. Comparing these with recent dynamical calculations involving gauge flux excitations and Majorana fermions of the pure Kitaev model, we propose the excitation spectrum of α-RuCl3 as a prime candidate for fractionalized Kitaev physics.

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Figure 1: Structure and bulk properties of 2D layered α-RuCl3.
Figure 2: Spin–orbit coupling mode in α-RuCl3, measured using inelastic neutron scattering at T = 5 K with incident energy Ei = 1.5 eV.
Figure 3: Collective magnetic modes measured with inelastic neutron scattering using 25 meV incident neutrons.
Figure 4: Spin wave theory calculations.
Figure 5: Disagreements with classical SWT and agreement with QSL calculations.

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Acknowledgements

Research using ORNL’s HFIR and SNS facilities was sponsored by the US Department of Energy, Office of Science, Basic Energy Sciences (BES), Scientific User Facilities Division. A part of the synthesis and the bulk characterization performed at ORNL was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (C.A.B. and J.-Q.Y.). The work at University of Tennessee was funded in part by the Gordon and Betty Moore Foundation’s EPiQS Initiative through Grant GBMF4416 (D.G.M. and L.L.). The work at Dresden was in part supported by DFG grant SFB 1143 (J.K. and R.M.), and by a fellowship within the Postdoc-Program of the German Academic Exchange Service (DAAD) (J.K.). D.L.K. is supported by EPSRC Grant No. EP/M007928/1. The collaboration as a whole was supported by the Helmholtz Virtual Institute ‘New States of Matter and their Excitations’ initiative. We thank B. Chakoumakos for overall support in the project, and J. Chalker, J. Rau, S. Toth, G. Khaliullin and F. Ye for valuable discussions. We thank P. Whitfield from the POWGEN beamline and Z. Gai from the CNMS facility for helping with neutron diffraction and magnetic susceptibility measurements.

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Authors and Affiliations

  1. Quantum Condensed Matter Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, USA

    A. Banerjee, A. A. Aczel, M. B. Stone, G. E. Granroth, M. D. Lumsden & S. E. Nagler

  2. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, USA

    C. A. Bridges

  3. Material Sciences and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, USA

    J.-Q. Yan & D. G. Mandrus

  4. Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, USA

    J.-Q. Yan & D. G. Mandrus

  5. Department of Physics, University of Tennessee, Knoxville, Tennessee 37996, USA

    L. Li & Y. Yiu

  6. Neutron Data Analysis & Visualization Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, USA

    G. E. Granroth

  7. Department of Physics, Cavendish Laboratory, J.J. Thomson Avenue, Cambridge CB3 0HE, UK

    J. Knolle & D. L. Kovrizhin

  8. Max Planck Institute for the Physics of Complex Systems, D-01187 Dresden, Germany

    S. Bhattacharjee & R. Moessner

  9. International Center for Theoretical Sciences, TIFR, Bangalore 560012, India

    S. Bhattacharjee

  10. Neutron Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, USA

    D. A. Tennant

  11. Bredesen Center, University of Tennessee, Knoxville, Tennessee 37966, USA

    S. E. Nagler

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  1. A. Banerjee
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Contributions

S.E.N., A.B. and D.G.M. conceived the project and the experiment. C.A.B., A.B., L.L., J.-Q.Y., Y.Y. and D.G.M. made the sample. J.-Q.Y., L.L., A.B. and C.A.B. performed the bulk measurements, A.B., A.A.A., M.B.S., G.E.G., M.D.L. and S.E.N. performed INS measurements, A.B., S.E.N., C.A.B., M.D.L., M.B.S. and D.A.T. analysed the data. Further modelling and interpreting of the neutron scattering data was carried out by A.B., M.D.L., S.E.N., J.K., S.B., D.L.K. and R.M., where A.B., M.D.L., S.B. and S.E.N. performed SWT simulations, and J.K., S.B., D.L.K. and R.M. carried out QSL theory calculations. A.B. and S.E.N. prepared the first draft, and all authors contributed to writing the manuscript.

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Correspondence to A. Banerjee or S. E. Nagler.

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Banerjee, A., Bridges, C., Yan, JQ. et al. Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet. Nature Mater 15, 733–740 (2016). https://doi.org/10.1038/nmat4604

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