Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3

Hwan Chun, Sae; Kim, Jong-Woo; Kim, Jungho; Zheng, H.; Stoumpos, Constantinos C.; Malliakas, C. D.; Mitchell, J. F.; Mehlawat, Kavita; Singh, Yogesh; Choi, Y.; Gog, T.; Al-Zein, A.; Sala, M. Moretti; Krisch, M.; Chaloupka, J.; Jackeli, G.; Khaliullin, G.; Kim, B. J.

doi:10.1038/nphys3322

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na₂IrO₃

Journal Article · Mon May 11 00:00:00 EDT 2015 · Nature Physics

DOI:https://doi.org/10.1038/nphys3322· OSTI ID:1355347

Hwan Chun, Sae ^[1]; Kim, Jong-Woo ^[2]; Kim, Jungho ^[2]; Zheng, H. ^[1]; Stoumpos, Constantinos C. ^[1]; Malliakas, C. D. ^[1]; Mitchell, J. F. ^[1]; Mehlawat, Kavita ^[3]; Singh, Yogesh ^[3]; Choi, Y. ^[2]; Gog, T. ^[2]; Al-Zein, A. ^[4]; Sala, M. Moretti ^[4]; Krisch, M. ^[4]; Chaloupka, J. ^[5]; Jackeli, G. ^[6]; Khaliullin, G. ^[7]; Kim, B. J. ^[7]

Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Indian Institute of Science Education and Research (IISER) Mohali, Knowledge City (India)
European Synchrotron Radiation Facility (France)
Masaryk University (Czech Republic). Central European Institute of Technology
Max Planck Institute for Solid State Research (Germany); University of Stuttgart (Germany). Institute for Functional Matter and Quantum Technologies
Max Planck Institute for Solid State Research (Germany)

We show that heisenberg interactions are ubiquitous in magnetic materials and play a central role in modelling and designing quantum magnets. Bond-directional interactions offer a novel alternative to Heisenberg exchange and provide the building blocks of the Kitaev model, which has a quantum spin liquid as its exact ground state. Honeycomb iridates, A₂IrO₃ (A = Na, Li), offer potential realizations of the Kitaev magnetic exchange coupling, and their reported magnetic behaviour may be interpreted within the Kitaev framework. However, the extent of their relevance to the Kitaev model remains unclear, as evidence for bond-directional interactions has so far been indirect. Here we present direct evidence for dominant bond-directional interactions in antiferromagnetic Na₂IrO₃ and show that they lead to strong magnetic frustration. Diffuse magnetic X-ray scattering reveals broken spin-rotational symmetry even above the Néel temperature, with the three spin components exhibiting short-range correlations along distinct crystallographic directions. Lastly, this spin- and real-space entanglement directly uncovers the bond-directional nature of these interactions, thus providing a direct connection between honeycomb iridates and Kitaev physics.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1355347

Journal Information:: Nature Physics, Journal Name: Nature Physics Journal Issue: 6 Vol. 11; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

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Topological magnons in Kitaev magnets at high fields McClarty, P. A.; Dong, X. -Y.; Gohlke, M. Physical Review B, Vol. 98, Issue 6 https://doi.org/10.1103/physrevb.98.060404	journal	August 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
Anisotropic susceptibilities in the honeycomb Kitaev system α − RuCl 3 Lampen-Kelley, P.; Rachel, S.; Reuther, J. Physical Review B, Vol. 98, Issue 10 https://doi.org/10.1103/physrevb.98.100403	journal	September 2018
Magnetic dynamics and spin-phonon coupling in the antiferromagnet Ni 2 NbBO 6 Prosnikov, M. A.; Smirnov, A. N.; Davydov, V. Yu. Physical Review B, Vol. 98, Issue 10 https://doi.org/10.1103/physrevb.98.104404	journal	September 2018
Spin-gap and two-dimensional magnetic excitations in Sr 2 IrO 4 Calder, S.; Pajerowski, D. M.; Stone, M. B. Physical Review B, Vol. 98, Issue 22 https://doi.org/10.1103/physrevb.98.220402	journal	December 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
Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr 2 IrO 4 Porras, J.; Bertinshaw, J.; Liu, H. Physical Review B, Vol. 99, Issue 8 https://doi.org/10.1103/physrevb.99.085125	journal	February 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
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
First-Principles Study of the Magnetic Structure of Na 2 IrO 3 Hu, Kaige; Wang, Fa; Feng, Ji Physical Review Letters, Vol. 115, Issue 16 https://doi.org/10.1103/physrevlett.115.167204	journal	October 2015
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
Honeycomb-Lattice Heisenberg-Kitaev Model in a Magnetic Field: Spin Canting, Metamagnetism, and Vortex Crystals Janssen, Lukas; Andrade, Eric C.; Vojta, Matthias Physical Review Letters, Vol. 117, Issue 27 https://doi.org/10.1103/physrevlett.117.277202	journal	December 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
Anomalous Thermal Conductivity and Magnetic Torque Response in the Honeycomb Magnet α − RuCl 3 Leahy, Ian A.; Pocs, Christopher A.; Siegfried, Peter E. Physical Review Letters, Vol. 118, Issue 18 https://doi.org/10.1103/physrevlett.118.187203	journal	May 2017
Two-Dimensional J eff = 1 / 2 Antiferromagnetic Insulator Unraveled from Interlayer Exchange Coupling in Artificial Perovskite Iridate Superlattices Hao, Lin; Meyers, D.; Frederick, Clayton Physical Review Letters, Vol. 119, Issue 2 https://doi.org/10.1103/physrevlett.119.027204	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
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
Quantization of the Thermal Hall Conductivity at Small Hall Angles Ye, Mengxing; Halász, Gábor B.; Savary, Lucile Physical Review Letters, Vol. 121, Issue 14 https://doi.org/10.1103/physrevlett.121.147201	journal	October 2018
Bond-Disordered Spin Liquid and the Honeycomb Iridate H 3 LiIr 2 O 6 : Abundant Low-Energy Density of States from Random Majorana Hopping Knolle, Johannes; Moessner, Roderich; Perkins, Natalia B. Physical Review Letters, Vol. 122, Issue 4 https://doi.org/10.1103/physrevlett.122.047202	journal	February 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
Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb 2 Si 2 O 7 Hester, Gavin; Nair, H. S.; Reeder, T. Physical Review Letters, Vol. 123, Issue 2 https://doi.org/10.1103/physrevlett.123.027201	journal	July 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
Possible Quantum Paramagnetism in Compressed Sr 2 IrO 4 Haskel, D.; Fabbris, G.; Kim, J. H. Physical Review Letters, Vol. 124, Issue 6 https://doi.org/10.1103/physrevlett.124.067201	journal	February 2020
Octupolar versus Néel Order in Cubic 5 d 2 Double Perovskites Maharaj, D. D.; Sala, G.; Stone, M. B. Physical Review Letters, Vol. 124, Issue 8 https://doi.org/10.1103/physrevlett.124.087206	journal	February 2020
Relativistic G W +BSE study of the optical properties of Ruddlesden-Popper iridates Liu, Peitao; Kim, Bongjae; Chen, Xing-Qiu Physical Review Materials, Vol. 2, Issue 7 https://doi.org/10.1103/physrevmaterials.2.075003	journal	July 2018
Dirac nodal lines protected against spin-orbit interaction in IrO 2 Nelson, J. N.; Ruf, J. P.; Lee, Y. Physical Review Materials, Vol. 3, Issue 6 https://doi.org/10.1103/physrevmaterials.3.064205	journal	June 2019
Steplike metamagnetic transitions in a honeycomb lattice antiferromagnet Tb 2 Ir 3 Ga 9 Khan, Mojammel A.; Zhang, Qiang; Bao, Jin-Ke Physical Review Materials, Vol. 3, Issue 11 https://doi.org/10.1103/physrevmaterials.3.114411	journal	November 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
Nonequilibrium Majorana dynamics by quenching a magnetic field in Kitaev spin liquids Nasu, Joji; Motome, Yukitoshi Physical Review Research, Vol. 1, Issue 3 https://doi.org/10.1103/physrevresearch.1.033007	journal	October 2019
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
Phase Diagram and Quantum Order by Disorder in the Kitaev K 1 − K 2 Honeycomb Magnet Rousochatzakis, Ioannis; Reuther, Johannes; Thomale, Ronny Physical Review X, Vol. 5, Issue 4 https://doi.org/10.1103/physrevx.5.041035	journal	December 2015
Spin Liquid State and Topological Structural Defects in Hexagonal TbInO 3 Kim, Jaewook; Wang, Xueyun; Huang, Fei-Ting Physical Review X, Vol. 9, Issue 3 https://doi.org/10.1103/physrevx.9.031005	journal	July 2019
A high-energy-resolution resonant inelastic X-ray scattering spectrometer at ID20 of the European Synchrotron Radiation Facility Moretti Sala, M.; Martel, K.; Henriquet, C. Journal of Synchrotron Radiation, Vol. 25, Issue 2 https://doi.org/10.1107/s1600577518001200	journal	February 2018
X-ray magnetic diffraction under high pressure Wang, Yishu; Rosenbaum, T. F.; Feng, Yejun IUCrJ, Vol. 6, Issue 4 https://doi.org/10.1107/s2052252519007061	journal	June 2019
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
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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
Spin Liquid versus Spin Orbit Coupling on the Triangular Lattice Iaconis, Jason; Liu, Chunxiao; Halász, Gábor SciPost Physics, Vol. 4, Issue 1 https://doi.org/10.21468/scipostphys.4.1.003	journal	January 2018
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Superconducting quantum simulator for topological order and the toric code Browne, Dan E.; Wallraff, Andreas; Hartmann, Michael J. ETH Zurich https://doi.org/10.3929/ethz-b-000196764	text	January 2017
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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
Honeycomb-lattice Heisenberg-Kitaev model in a magnetic field: Spin canting, metamagnetism, and vortex crystals Janssen, Lukas; Andrade, Eric C.; Vojta, Matthias arXiv https://doi.org/10.48550/arxiv.1607.04640	text	January 2016
Spin Liquid versus Spin Orbit Coupling on the Triangular Lattice Iaconis, Jason; Liu, Chunxiao; Halász, Gábor B. arXiv https://doi.org/10.48550/arxiv.1708.07856	text	January 2017
Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates Paramekanti, Arun; Singh, David J.; Yuan, Bo arXiv https://doi.org/10.48550/arxiv.1804.02006	text	January 2018
Quantization of the thermal Hall conductivity at small Hall angles Ye, Mengxing; Halász, Gábor B.; Savary, Lucile arXiv https://doi.org/10.48550/arxiv.1805.10532	text	January 2018
Relativistic $GW$+BSE study of the optical properties of Ruddlesden-Popper iridates Liu, Peitao; Kim, Bongjae; Chen, Xing-Qiu arXiv https://doi.org/10.48550/arxiv.1806.07280	text	January 2018
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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
Quantum Spin Liquids Broholm, C.; Cava, R. J.; Kivelson, S. A. arXiv https://doi.org/10.48550/arxiv.1905.07040	text	January 2019
Nonequilibrium Majorana Dynamics by Quenching a Magnetic Field in Kitaev Spin Liquids Nasu, Joji; Motome, Yukitoshi arXiv https://doi.org/10.48550/arxiv.1905.10984	text	January 2019

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