Field evolution of magnons in α-RuCl3 by high-resolution polarized terahertz spectroscopy

Wu, Liang; Little, A.; Aldape, E. E.; Rees, D.; Thewalt, E.; Lampen-Kelley, P.; Banerjee, A.; Bridges, C. A.; Yan, J. -Q.; Boone, D.; Patankar, S.; Goldhaber-Gordon, D.; Mandrus, D.; Nagler, S. E.; Altman, E.; Orenstein, J.

doi:10.1103/physrevb.98.094425

Title: Field evolution of magnons in $α - {RuCl}_{3}$ by high-resolution polarized terahertz spectroscopy

Journal Article · 25 September 2018 · Physical Review B

DOI: https://doi.org/10.1103/physrevb.98.094425 · OSTI ID:1562881

Wu, Liang ^[1]; Little, A. ^[2]; Aldape, E. E. ^[3]; Rees, D. ^[2]; Thewalt, E. ^[2]; Lampen-Kelley, P. ^[4]; Banerjee, A. ^[5]; Bridges, C. A. ^[5]; Yan, J. -Q. ^[5]; Boone, D. ^[6]; Patankar, S. ^[2]; Goldhaber-Gordon, D. ^[6]; Mandrus, D. ^[4]; Nagler, S. E. ^[5]; Altman, E. ^[3]; Orenstein, J. ^[2]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Pennsylvania, Philadelphia, PA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Here, the Kitaev quantum spin liquid (KSL) is a theoretically predicted state of matter whose fractionalized quasiparticles are distinct from bosonic magnons, the fundamental excitation in ordered magnets. The layered honeycomb antiferromagnet α–RuCl₃ is a KSL candidate material, as it can be driven to a magnetically disordered phase by application of an in-plane magnetic field, with H_c ~ 7 T. Here, we report a detailed characterization of the magnetic excitation spectrum of this material by high-resolution time-domain terahertz spectroscopy. We observe two sharp magnon resonances whose frequencies and amplitudes exhibit a discontinuity as a function of applied magnetic field, as well as two broader peaks at higher energy. Below the Néel temperature, we find that linear spin wave theory can account for all of these essential features of the spectra when a C₃-breaking distortion of the honeycomb lattice and the presence of structural domains are taken into account.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Gordon and Betty Moore Foundation

Grant/Contract Number:: AC02-05CH11231; AC02-05CH11231; AC02-76SF00515; AC05-00OR22725

OSTI ID:: 1562881

Alternate ID(s):: OSTI ID: 1761765; OSTI ID: 1474001

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 9 Vol. 98; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (59)

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
α − RuCl 3 : A spin-orbit assisted Mott insulator on a honeycomb lattice Plumb, K. W.; Clancy, J. P.; Sandilands, L. J. Physical Review B, Vol. 90, Issue 4 https://doi.org/10.1103/PhysRevB.90.041112	journal	July 2014
Mechanism for subgap optical conductivity in honeycomb Kitaev materials Bolens, Adrien; Katsura, Hosho; Ogata, Masao arXiv https://doi.org/10.48550/arxiv.1711.00308	text	January 2017
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models Jackeli, G.; Khaliullin, G. Physical Review Letters, Vol. 102, Issue 1 https://doi.org/10.1103/PhysRevLett.102.017205	journal	January 2009
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
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
Kitaev magnetism in honeycomb RuCl 3 with intermediate spin-orbit coupling Kim, Heung-Sik; V., Vijay Shankar; Catuneanu, Andrei Physical Review B, Vol. 91, Issue 24 https://doi.org/10.1103/PhysRevB.91.241110	journal	June 2015
Field Dependence of the Intrinsic Domain Magnetization of a Ferromagnet Holstein, T.; Primakoff, H. Physical Review, Vol. 58, Issue 12 https://doi.org/10.1103/PhysRev.58.1098	journal	December 1940
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
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
Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales Winter, Stephen M.; Li, Ying; Jeschke, Harald O. Physical Review B, Vol. 93, Issue 21 https://doi.org/10.1103/PhysRevB.93.214431	journal	June 2016
Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young Physical Review Letters, Vol. 112, Issue 7 https://doi.org/10.1103/PhysRevLett.112.077204	journal	February 2014
Atomic-scale observation of structural and electronic orders in the layered compound α-RuCl3 Ziatdinov, M.; Banerjee, A.; Maksov, A. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13774	journal	December 2016
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
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
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
Electronic and phonon excitations in α − RuC l 3 Reschke, S.; Mayr, F.; Wang, Zhe Physical Review B, Vol. 96, Issue 16 https://doi.org/10.1103/PhysRevB.96.165120	journal	October 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
Emergent phenomena induced by spin–orbit coupling at surfaces and interfaces Soumyanarayanan, Anjan; Reyren, Nicolas; Fert, Albert Nature, Vol. 539, Issue 7630 https://doi.org/10.1038/nature19820	journal	November 2016
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
Long-range magnetic ordering in Na 2 IrO 3 Liu, X.; Berlijn, T.; Yin, W. -G. Physical Review B, Vol. 83, Issue 22 https://doi.org/10.1103/PhysRevB.83.220403	journal	June 2011
Incommensurate counterrotating magnetic order stabilized by Kitaev interactions in the layered honeycomb α − Li 2 IrO 3 Williams, S. C.; Johnson, R. D.; Freund, F. Physical Review B, Vol. 93, Issue 19 https://doi.org/10.1103/PhysRevB.93.195158	journal	May 2016
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
Generic spin model for the honeycomb iridates beyond the Kitaev limit Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young arXiv https://doi.org/10.48550/arxiv.1310.7940	text	January 2013
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
Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid Kasahara, Y.; Ohnishi, T.; Mizukami, Y. Nature, Vol. 559, Issue 7713 https://doi.org/10.1038/s41586-018-0274-0	journal	July 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
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
Low-temperature crystal and magnetic structure of α − RuCl 3 Cao, H. B.; Banerjee, A.; Yan, J. -Q. Physical Review B, Vol. 93, Issue 13 https://doi.org/10.1103/PhysRevB.93.134423	journal	April 2016
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
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
Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in γ − Li 2 IrO 3 Biffin, A.; Johnson, R. D.; Kimchi, I. Physical Review Letters, Vol. 113, Issue 19 https://doi.org/10.1103/PhysRevLett.113.197201	journal	November 2014
Fault-tolerant quantum computation by anyons Kitaev, A. Yu. Annals of Physics, Vol. 303, Issue 1 https://doi.org/10.1016/S0003-4916(02)00018-0	journal	January 2003
Diagonalization of the quadratic boson hamiltonian Colpa, J. H. P. Physica A: Statistical Mechanics and its Applications, Vol. 93, Issue 3-4 https://doi.org/10.1016/0378-4371(78)90160-7	journal	September 1978
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
Magnetic thermal conductivity far above the Néel temperature in the Kitaev-magnet candidate α − RuCl 3 Hirobe, Daichi; Sato, Masahiro; Shiomi, Yuki Physical Review B, Vol. 95, Issue 24 https://doi.org/10.1103/PhysRevB.95.241112	journal	June 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
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
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
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
Scanning X-ray microdiffraction with submicrometer white beam for strain/stress and orientation mapping in thin films Tamura, N.; MacDowell, A. A.; Spolenak, R. Journal of Synchrotron Radiation, Vol. 10, Issue 2 https://doi.org/10.1107/S0909049502021362	journal	February 2003
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
Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 Hwan Chun, Sae; Kim, Jong-Woo; Kim, Jungho Nature Physics, Vol. 11, Issue 6 https://doi.org/10.1038/nphys3322	journal	May 2015
Magnetic order in α − RuCl 3 : A honeycomb-lattice quantum magnet with strong spin-orbit coupling Sears, J. A.; Songvilay, M.; Plumb, K. W. Physical Review B, Vol. 91, Issue 14 https://doi.org/10.1103/PhysRevB.91.144420	journal	April 2015
Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate Modic, K. A.; Smidt, Tess E.; Kimchi, Itamar Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5203	journal	June 2014
Mechanism for subgap optical conductivity in honeycomb Kitaev materials Bolens, Adrien; Katsura, Hosho; Ogata, Masao Physical Review B, Vol. 97, Issue 16 https://doi.org/10.1103/PhysRevB.97.161108	journal	April 2018
Monoclinic crystal structure of α − RuCl 3 and the zigzag antiferromagnetic ground state Johnson, R. D.; Williams, S. C.; Haghighirad, A. A. Physical Review B, Vol. 92, Issue 23 https://doi.org/10.1103/PhysRevB.92.235119	journal	December 2015
Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3 Yadav, Ravi; Bogdanov, Nikolay A.; Katukuri, Vamshi M. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep37925	journal	November 2016
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
Fault-tolerant quantum computation by anyons Kitaev, A. Yu. arXiv https://doi.org/10.48550/arxiv.quant-ph/9707021	text	January 1997
Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides A 2 IrO 3 Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat Physical Review Letters, Vol. 105, Issue 2 https://doi.org/10.1103/PhysRevLett.105.027204	journal	July 2010
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
Anyons in an exactly solved model and beyond Kitaev, Alexei arXiv https://doi.org/10.48550/arxiv.cond-mat/0506438	text	January 2005
Linear spin wave theory for single-Q incommensurate magnetic structures Toth, S.; Lake, B. arXiv https://doi.org/10.48550/arxiv.1402.6069	text	January 2014
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
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
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
Hyperhoneycomb Iridate β − Li 2 IrO 3 as a Platform for Kitaev Magnetism Takayama, T.; Kato, A.; Dinnebier, R. Physical Review Letters, Vol. 114, Issue 7 https://doi.org/10.1103/PhysRevLett.114.077202	journal	February 2015

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Dynamical and thermal magnetic properties of the Kitaev spin liquid candidate α-RuCl3 Laurell, Pontus; Okamoto, Satoshi npj Quantum Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41535-019-0203-y	journal	January 2020
Sub-gap optical response in the Kitaev spin-liquid candidate α -RuCl ₃ Reschke, Stephan; Mayr, Franz; Widmann, Sebastian Journal of Physics: Condensed Matter, Vol. 30, Issue 47 https://doi.org/10.1088/1361-648x/aae805	journal	November 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
Two-step gap opening across the quantum critical point in the Kitaev honeycomb magnet α − RuCl 3 Nagai, Yuya; Jinno, Takaaki; Yoshitake, Junki Physical Review B, Vol. 101, Issue 2 https://doi.org/10.1103/physrevb.101.020414	journal	January 2020
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