Cobalt-based pyroxenes: A new playground for Kitaev physics

Maksimov, Pavel A.; Ushakov, Alexey V.; Gubkin, Andrey F.; Redhammer, Günther J.; Winter, Stephen M.; Kolesnikov, Alexander I.; dos Santos, Antonio M.; Gai, Zheng; McGuire, Michael A.; Podlesnyak, Andrey; Streltsov, Sergey V.

doi:10.1073/pnas.2409154121

Title: Cobalt-based pyroxenes: A new playground for Kitaev physics

Journal Article · 18 October 2024 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.2409154121 · OSTI ID:2474768

^[1];

^[2];

^[3]; Redhammer, Günther J. ^[4]; Winter, Stephen M. ^[5];

^[6];

^[7];

^[6];

^[3]

Joint Institute for Nuclear Research, Dubna (Russian Federation); Russian Academy of Sciences (RAS) Ural Branch, Moscow (Russian Federation). M. N. Miheev Institute of Metal Physics
Russian Academy of Sciences (RAS) Ural Branch, Moscow (Russian Federation). M. N. Miheev Institute of Metal Physics
Russian Academy of Sciences (RAS) Ural Branch, Moscow (Russian Federation). M. N. Miheev Institute of Metal Physics; Ural Federal Univ., Ekaterinburg (Russian Federation)
University of Salzburg (Austria)
Wake Forest Univ., Winston-Salem, NC (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Recent advances in the study of cobaltites have unveiled their potential as a promising platform for realizing Kitaev physics in honeycomb systems and the Ising model in weakly coupled chain materials. In this manuscript, we explore the magnetic properties of pyroxene SrCoGe₂O₆ using a combination of neutron scattering, ab initio methods, and linear spin-wave theory. Through careful examination of inelastic neutron scattering powder spectra, we propose a modified Kitaev model to accurately describe the twisted chains of edge-sharing octahedra surrounding Co²⁺ ions. The extended Kitaev–Heisenberg model, including a significant anisotropic bond-dependent exchange term with K/|J| = 0.96, is identified as the key descriptor of the magnetic interactions in SrCoGe₂O₆. Furthermore, our heat capacity measurements reveal an effect of an external magnetic field (approximately 13 T) which shifts the system from a fragile antiferromagnetic ordering with T_N = 9 K to a field-induced state. We argue that pyroxenes, particularly those modified by substituting Ge with Si and its less extended p orbitals, emerge as a platform for the Kitaev model. This opens up possibilities for advancing our understanding of Kitaev physics.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2474768

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 43 Vol. 121; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

References (66)

Role of the transition zone and 660 km discontinuity in mantle dynamics Ringwood, A. E. Physics of the Earth and Planetary Interiors, Vol. 86, Issue 1-3 https://doi.org/10.1016/0031-9201(94)05058-9	journal	October 1994
What is the spin of a spin wave? Faddeev, L. D.; Takhtajan, L. A. Physics Letters A, Vol. 85, Issue 6-7 https://doi.org/10.1016/0375-9601(81)90335-2	journal	October 1981
Anyons in an exactly solved model and beyond Kitaev, Alexei Annals of Physics, Vol. 321, Issue 1 https://doi.org/10.1016/j.aop.2005.10.005	journal	January 2006
Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments Arnold, O.; Bilheux, J. C.; Borreguero, J. M. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764 https://doi.org/10.1016/j.nima.2014.07.029	journal	November 2014
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet Banerjee, A.; Bridges, C. A.; Yan, J. -Q. Nature Materials, Vol. 15, Issue 7 https://doi.org/10.1038/nmat4604	journal	April 2016
Interplay of quantum criticality and geometric frustration in columbite Lee, SungBin; Kaul, Ribhu K.; Balents, Leon Nature Physics, Vol. 6, Issue 9 https://doi.org/10.1038/nphys1696	journal	June 2010
Breakdown of magnons in a strongly spin-orbital coupled magnet Winter, Stephen M.; Riedl, Kira; Maksimov, Pavel A. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-01177-0	journal	October 2017
Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition Bozin, E. S.; Yin, W. G.; Koch, R. J. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11372-w	journal	August 2019
Magnon bound states versus anyonic Majorana excitations in the Kitaev honeycomb magnet α-RuCl3 Wulferding, Dirk; Choi, Youngsu; Do, Seung-Hwan Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15370-1	journal	March 2020
Order-by-disorder from bond-dependent exchange and intensity signature of nodal quasiparticles in a honeycomb cobaltate Elliot, M.; McClarty, P. A.; Prabhakaran, D. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23851-0	journal	June 2021
Field-induced quantum spin disordered state in spin-1/2 honeycomb magnet Na2Co2TeO6 Lin, Gaoting; Jeong, Jaehong; Kim, Chaebin Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-25567-7	journal	September 2021
Excitations in the field-induced quantum spin liquid state of α-RuCl3 Banerjee, Arnab; Lampen-Kelley, Paula; Knolle, Johannes npj Quantum Materials, Vol. 3, Issue 1 https://doi.org/10.1038/s41535-018-0079-2	journal	February 2018
Duality and domain wall dynamics in a twisted Kitaev chain Morris, C. M.; Desai, Nisheeta; Viirok, J. Nature Physics, Vol. 17, Issue 7 https://doi.org/10.1038/s41567-021-01208-0	journal	April 2021
Concept and realization of Kitaev quantum spin liquids Takagi, Hidenori; Takayama, Tomohiro; Jackeli, George Nature Reviews Physics, Vol. 1, Issue 4 https://doi.org/10.1038/s42254-019-0038-2	journal	March 2019
SrMGe ₂ O ₆ (M = Mn, Co): a family of pyroxene compounds displaying multiferroicity Ding, Lei; Colin, Claire V.; Darie, Céline Journal of Materials Chemistry C, Vol. 4, Issue 19 https://doi.org/10.1039/C6TC00149A	journal	January 2016
The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance Ehlers, G.; Podlesnyak, A. A.; Niedziela, J. L. Review of Scientific Instruments, Vol. 82, Issue 8 https://doi.org/10.1063/1.3626935	journal	August 2011
The cold neutron chopper spectrometer at the Spallation Neutron Source—A review of the first 8 years of operation Ehlers, G.; Podlesnyak, A. A.; Kolesnikov, A. I. Review of Scientific Instruments, Vol. 87, Issue 9 https://doi.org/10.1063/1.4962024	journal	September 2016
Katanin, Andrei A.; Katanin, Andrei A.; Irkhin, Valentin Yu. Physics-Uspekhi, Vol. 50, Issue 6 https://doi.org/10.1070/PU2007v050n06ABEH006313	journal	January 2007
Glide symmetry breaking and Ising criticality in the quasi-1D magnet CoNb ₂ O ₆ Fava, Michele; Coldea, Radu; Parameswaran, S. A. Proceedings of the National Academy of Sciences, Vol. 117, Issue 41 https://doi.org/10.1073/pnas.2007986117	journal	September 2020
Pyroxenes: a new class of multiferroics Jodlauk, S.; Becker, P.; Mydosh, J. A. Journal of Physics: Condensed Matter, Vol. 19, Issue 43 https://doi.org/10.1088/0953-8984/19/43/432201	journal	September 2007
Linear spin wave theory for single-Q incommensurate magnetic structures Toth, S.; Lake, B. Journal of Physics: Condensed Matter, Vol. 27, Issue 16 https://doi.org/10.1088/0953-8984/27/16/166002	journal	March 2015
Models and materials for generalized Kitaev magnetism Winter, Stephen M.; Tsirlin, Alexander A.; Daghofer, Maria Journal of Physics: Condensed Matter, Vol. 29, Issue 49 https://doi.org/10.1088/1361-648X/aa8cf5	journal	November 2017
Antiferromagnetic Kitaev interaction inJ _eff = 1/2 cobalt honeycomb materials Na ₃ Co ₂ SbO ₆ and Na ₂ Co ₂ TeO ₆ Kim, Chaebin; Jeong, Jaehong; Lin, Gaoting Journal of Physics: Condensed Matter, Vol. 34, Issue 4 https://doi.org/10.1088/1361-648X/ac2644	journal	November 2021
SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS Granroth, G. E.; Kolesnikov, A. I.; Sherline, T. E. Journal of Physics: Conference Series, Vol. 251 https://doi.org/10.1088/1742-6596/251/1/012058	journal	November 2010
Magnetic couplings in edge-sharing high-spin d ⁷ compounds Winter, Stephen M. Journal of Physics: Materials, Vol. 5, Issue 4 https://doi.org/10.1088/2515-7639/ac94f8	journal	October 2022
Theory of Dipole Interaction in Crystals Luttinger, J. M.; Tisza, L. Physical Review, Vol. 70, Issue 11-12 https://doi.org/10.1103/PhysRev.70.954	journal	December 1946
High-field quantum disordered state in α − RuCl 3 : Spin flips, bound states, and multiparticle continuum Sahasrabudhe, A.; Kaib, D. A. S.; Reschke, S. Physical Review B, Vol. 101, Issue 14 https://doi.org/10.1103/PhysRevB.101.140410	journal	April 2020
Kitaev interactions in the Co honeycomb antiferromagnets Na 3 Co 2 SbO 6 and Na 2 Co 2 TeO 6 Songvilay, M.; Robert, J.; Petit, S. Physical Review B, Vol. 102, Issue 22 https://doi.org/10.1103/PhysRevB.102.224429	journal	December 2020
High-field thermal transport properties of the Kitaev quantum magnet α − Ru Cl 3 : Evidence for low-energy excitations beyond the critical field Hentrich, Richard; Hong, Xiaochen; Gillig, Matthias Physical Review B, Vol. 102, Issue 23 https://doi.org/10.1103/PhysRevB.102.235155	journal	December 2020
Modified Curie-Weiss law for j eff magnets Li, Ying; Winter, Stephen M.; Kaib, David A. S. Physical Review B, Vol. 103, Issue 22 https://doi.org/10.1103/PhysRevB.103.L220408	journal	June 2021
Static and dynamic magnetic properties of honeycomb lattice antiferromagnets Na2M2TeO6 , M=Co and Ni Samarakoon, Anjana M.; Chen, Qiang; Zhou, Haidong Physical Review B, Vol. 104, Issue 18 https://doi.org/10.1103/PhysRevB.104.184415	journal	November 2021
Single-ion properties of the transverse-field Ising model material CoNb2O6 Ringler, J. A.; Kolesnikov, A. I.; Ross, K. A. Physical Review B, Vol. 105, Issue 22 https://doi.org/10.1103/PhysRevB.105.224421	journal	June 2022
Dominant Kitaev interactions in the honeycomb materials Na3Co2SbO6 and Na2Co2TeO6 Sanders, Alaric L.; Mole, Richard A.; Liu, Jiatu Physical Review B, Vol. 106, Issue 1 https://doi.org/10.1103/PhysRevB.106.014413	journal	July 2022
Ab initio guided minimal model for the “Kitaev” material BaCo2 ( AsO4)2 : Importance of direct hopping, third-neighbor exchange, and quantum fluctuations Maksimov, Pavel A.; Ushakov, Alexey V.; Pchelkina, Zlata V. Physical Review B, Vol. 106, Issue 16 https://doi.org/10.1103/PhysRevB.106.165131	journal	October 2022
Easy-plane anisotropic-exchange magnets on a honeycomb lattice: Quantum effects and dealing with them Maksimov, P. A.; Chernyshev, A. L. Physical Review B, Vol. 106, Issue 21 https://doi.org/10.1103/PhysRevB.106.214411	journal	December 2022
Magnetic phase diagram and possible Kitaev-like behavior of the honeycomb-lattice antimonate Na3Co2SbO6 Vavilova, E.; Vasilchikova, T.; Vasiliev, A. Physical Review B, Vol. 107, Issue 5 https://doi.org/10.1103/PhysRevB.107.054411	journal	February 2023
Non-Kitaev versus Kitaev honeycomb cobaltates Liu, Xiaoyu; Kee, Hae-Young Physical Review B, Vol. 107, Issue 5 https://doi.org/10.1103/PhysRevB.107.054420	journal	February 2023
Excitations of quantum Ising chain CoNb2O6 in low transverse field: Quantitative description of bound states stabilized by off-diagonal exchange and applied field Woodland, Leonie; Lovas, Izabella; Telling, M. Physical Review B, Vol. 108, Issue 18 https://doi.org/10.1103/PhysRevB.108.184417	journal	November 2023
Magnon interactions in the quantum paramagnetic phase of CoNb2O6 Gallegos, C. A.; Chernyshev, A. L. Physical Review B, Vol. 109, Issue 1 https://doi.org/10.1103/PhysRevB.109.014424	journal	January 2024
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators Liechtenstein, A. I.; Anisimov, V. I.; Zaanen, J. Physical Review B, Vol. 52, Issue 8 https://doi.org/10.1103/PhysRevB.52.R5467	journal	August 1995
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Quantum phase transition in the one-dimensional compass model Brzezicki, Wojciech; Dziarmaga, Jacek; Oleś, Andrzej M. Physical Review B, Vol. 75, Issue 13 https://doi.org/10.1103/PhysRevB.75.134415	journal	April 2007
Electronic structure and magnetic properties of pyroxenes ( Li , Na ) TM ( Si , Ge ) 2 O 6 : Low-dimensional magnets with 90° bonds Streltsov, S. V.; Khomskii, D. I. Physical Review B, Vol. 77, Issue 6 https://doi.org/10.1103/PhysRevB.77.064405	journal	February 2008
Successive magnetic phase transitions in α − RuCl 3 : XY-like frustrated magnet on the honeycomb lattice Kubota, Yumi; Tanaka, Hidekazu; Ono, Toshio Physical Review B, Vol. 91, Issue 9 https://doi.org/10.1103/PhysRevB.91.094422	journal	March 2015
Hidden symmetries of the extended Kitaev-Heisenberg model: Implications for the honeycomb-lattice iridates A 2 IrO 3 Chaloupka, Jiří; Khaliullin, Giniyat Physical Review B, Vol. 92, Issue 2 https://doi.org/10.1103/PhysRevB.92.024413	journal	July 2015
Pseudospin exchange interactions in d 7 cobalt compounds: Possible realization of the Kitaev model Liu, Huimei; Khaliullin, Giniyat Physical Review B, Vol. 97, Issue 1 https://doi.org/10.1103/PhysRevB.97.014407	journal	January 2018
Kitaev-Heisenberg Hamiltonian for high-spin d 7 Mott insulators Sano, Ryoya; Kato, Yasuyuki; Motome, Yukitoshi Physical Review B, Vol. 97, Issue 1 https://doi.org/10.1103/PhysRevB.97.014408	journal	January 2018
Spin-wave analysis of the low-temperature thermal Hall effect in the candidate Kitaev spin liquid α − RuCl 3 Cookmeyer, Jonathan; Moore, Joel E. Physical Review B, Vol. 98, Issue 6 https://doi.org/10.1103/PhysRevB.98.060412	journal	August 2018
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
Spin Waves and Revised Crystal Structure of Honeycomb Iridate Na 2 IrO 3 Choi, S. K.; Coldea, R.; Kolmogorov, A. N. Physical Review Letters, Vol. 108, Issue 12 https://doi.org/10.1103/PhysRevLett.108.127204	journal	March 2012
Scattering Continuum and Possible Fractionalized Excitations in α − RuCl 3 Sandilands, Luke J.; Tian, Yao; Plumb, Kemp W. Physical Review Letters, Vol. 114, Issue 14 https://doi.org/10.1103/PhysRevLett.114.147201	journal	April 2015
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
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
Absence of Ferromagnetism or Antiferromagnetism in One- or Two-Dimensional Isotropic Heisenberg Models Mermin, N. D.; Wagner, H. Physical Review Letters, Vol. 17, Issue 22 https://doi.org/10.1103/PhysRevLett.17.1133	journal	November 1966
Nonlinear Field Theory of Large-Spin Heisenberg Antiferromagnets: Semiclassically Quantized Solitons of the One-Dimensional Easy-Axis Néel State Haldane, F. D. M. Physical Review Letters, Vol. 50, Issue 15 https://doi.org/10.1103/PhysRevLett.50.1153	journal	April 1983
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevLett.78.1396	journal	February 1997
Comment on “Sodium Pyroxene NaTiSi 2 O 6 : Possible Haldane Spin-1 Chain System” Streltsov, S. V.; Popova, O. A.; Khomskii, D. I. Physical Review Letters, Vol. 96, Issue 24 https://doi.org/10.1103/PhysRevLett.96.249701	journal	June 2006
Topological Characterization of Quantum Phase Transitions in a Spin- 1 / 2 Model Feng, Xiao-Yong; Zhang, Guang-Ming; Xiang, Tao Physical Review Letters, Vol. 98, Issue 8 https://doi.org/10.1103/PhysRevLett.98.087204	journal	February 2007
Comprehensive study of the phase diagram of the spin- 12 Kitaev-Heisenberg-Gamma chain Yang, Wang; Nocera, Alberto; Affleck, Ian Physical Review Research, Vol. 2, Issue 3 https://doi.org/10.1103/PhysRevResearch.2.033268	journal	August 2020
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
Quantum Criticality in an Ising Chain: Experimental Evidence for Emergent E ₈ Symmetry Coldea, R.; Tennant, D. A.; Wheeler, E. M. Science, Vol. 327, Issue 5962 https://doi.org/10.1126/science.1180085	journal	January 2010
Orbital-assisted Peierls state in NaTiSi ₂ O ₆ Wezel, J. van; Brink, J. van den Europhysics Letters (EPL), Vol. 75, Issue 6 https://doi.org/10.1209/epl/i2006-10197-2	journal	September 2006
Spin Hamiltonians in Magnets: Theories and Computations Li, Xueyang; Yu, Hongyu; Lou, Feng Molecules, Vol. 26, Issue 4 https://doi.org/10.3390/molecules26040803	journal	February 2021
DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6 https://doi.org/10.6028/jres.114.025	journal	November 2009

Similar Records

Unusual Phonon Heat Transport in α-RuCl₃: Strong Spin-Phonon Scattering and Field-Induced Spin Gap

Journal Article · 2018 · Physical Review Letters · OSTI ID:1761763

Hentrich, Richard; Wolter, Anja U. B.; Zotos, Xenophon; +12 more

Destabilization of Magnetic Order in a Dilute Kitaev Spin Liquid Candidate

Journal Article · 2017 · Physical Review Letters · OSTI ID:1413606

Lampen-Kelley, Paige; Banerjee, Arnab; Aczel, Adam A.; +6 more

Static and dynamical magnetic properties of the extended Kitaev-Heisenberg model with spin vacancies

Journal Article · 2023 · Physical Review. B · OSTI ID:1996663

Li, Shaozhi; Fishman, Randy S.; Berlijn, Tom

Related Subjects

36 MATERIALS SCIENCE
Kitaev model
frustrated magnetism
inelastic neutron scattering
pyroxenes

Title: Cobalt-based pyroxenes: A new playground for Kitaev physics

Citation Formats

References (66)

Similar Records

Related Subjects