Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3
Abstract
The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we detect anomalous phonon effects in α-RuCl3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, JK~8 meV, that coincides with a giant acoustic phonon softening near the Z2 gauge flux energy scale. These phonon anomalies signify the coupling of phonon and Kitaev magnetic excitations in α-RuCl3 and demonstrates a proof-of-principle method to detect anomalous excitations in topological quantum materials.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Tokyo Institute of Technology (Japan)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Gordon and Betty Moore Foundation; Japan Society for the Promotion of Science (JSPS)
- OSTI Identifier:
- 1787494
- Alternate Identifier(s):
- OSTI ID: 1782548; OSTI ID: 1805025
- Report Number(s):
- BNL-221379-2021-JAAM
Journal ID: ISSN 2041-1723; 161217
- Grant/Contract Number:
- AC02-06CH11357; SC0012704; 21K13865; JP18H03678; GBMF9069; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Inelastic x-ray scattering; Kitaev quantum spin liquid; RuCl3; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Magnetic properties and materials; Quantum fluids and solids
Citation Formats
Li, Haoxiang, Zhang, Tiantian, Said, A. H., Fabbris, Gilberto, Mazzone, Daniel G., Yan, Jiaqiang, Mandrus, David, Halász, Gábor B., Okamoto, Satoshi, Murakami, S., Dean, M. P. M., Lee, Ho Nyung, and Miao, Hu. Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3. United States: N. p., 2021.
Web. doi:10.1038/s41467-021-23826-1.
Li, Haoxiang, Zhang, Tiantian, Said, A. H., Fabbris, Gilberto, Mazzone, Daniel G., Yan, Jiaqiang, Mandrus, David, Halász, Gábor B., Okamoto, Satoshi, Murakami, S., Dean, M. P. M., Lee, Ho Nyung, & Miao, Hu. Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3. United States. https://doi.org/10.1038/s41467-021-23826-1
Li, Haoxiang, Zhang, Tiantian, Said, A. H., Fabbris, Gilberto, Mazzone, Daniel G., Yan, Jiaqiang, Mandrus, David, Halász, Gábor B., Okamoto, Satoshi, Murakami, S., Dean, M. P. M., Lee, Ho Nyung, and Miao, Hu. Thu .
"Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3". United States. https://doi.org/10.1038/s41467-021-23826-1. https://www.osti.gov/servlets/purl/1787494.
@article{osti_1787494,
title = {Giant phonon anomalies in the proximate Kitaev quantum spin liquid α-RuCl3},
author = {Li, Haoxiang and Zhang, Tiantian and Said, A. H. and Fabbris, Gilberto and Mazzone, Daniel G. and Yan, Jiaqiang and Mandrus, David and Halász, Gábor B. and Okamoto, Satoshi and Murakami, S. and Dean, M. P. M. and Lee, Ho Nyung and Miao, Hu},
abstractNote = {The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we detect anomalous phonon effects in α-RuCl3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, JK~8 meV, that coincides with a giant acoustic phonon softening near the Z2 gauge flux energy scale. These phonon anomalies signify the coupling of phonon and Kitaev magnetic excitations in α-RuCl3 and demonstrates a proof-of-principle method to detect anomalous excitations in topological quantum materials.},
doi = {10.1038/s41467-021-23826-1},
journal = {Nature Communications},
number = 1,
volume = 12,
place = {United States},
year = {Thu Jun 10 00:00:00 EDT 2021},
month = {Thu Jun 10 00:00:00 EDT 2021}
}
Works referenced in this record:
Breakdown of magnons in a strongly spin-orbital coupled magnet
journal, October 2017
- Winter, Stephen M.; Riedl, Kira; Maksimov, Pavel A.
- Nature Communications, Vol. 8, Issue 1
Charge Friedel oscillations in a Mott insulator
journal, July 2011
- Mross, David F.; Senthil, T.
- Physical Review B, Vol. 84, Issue 4
High-Temperature Fractional Quantum Hall States
journal, June 2011
- Tang, Evelyn; Mei, Jia-Wei; Wen, Xiao-Gang
- Physical Review Letters, Vol. 106, Issue 23
Terahertz excitations in : Majorana fermions and rigid-plane shear and compression modes
journal, September 2019
- Reschke, S.; Tsurkan, V.; Do, S. -H.
- Physical Review B, Vol. 100, Issue 10
Neutron-scattering investigations of the Kohn anomaly and of the phase and amplitude charge-density-wave excitations of the blue bronze
journal, April 1991
- Pouget, J. P.; Hennion, B.; Escribe-Filippini, C.
- Physical Review B, Vol. 43, Issue 10
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016
- Banerjee, A.; Bridges, C. A.; Yan, J. -Q.
- Nature Materials, Vol. 15, Issue 7
Concept and realization of Kitaev quantum spin liquids
journal, March 2019
- Takagi, Hidenori; Takayama, Tomohiro; Jackeli, George
- Nature Reviews Physics, Vol. 1, Issue 4
Anyons in an exactly solved model and beyond
journal, January 2006
- Kitaev, Alexei
- Annals of Physics, Vol. 321, Issue 1
Quantum spin liquids
journal, January 2020
- Broholm, C.; Cava, R. J.; Kivelson, S. A.
- Science, Vol. 367, Issue 6475
Fermionic response from fractionalization in an insulating two-dimensional magnet
journal, July 2016
- Nasu, J.; Knolle, J.; Kovrizhin, D. L.
- Nature Physics, Vol. 12, Issue 10
Emergence of a field-driven U(1) spin liquid in the Kitaev honeycomb model
journal, January 2019
- Hickey, Ciarán; Trebst, Simon
- Nature Communications, Vol. 10, Issue 1
Unusual Thermal Hall Effect in a Kitaev Spin Liquid Candidate
journal, May 2018
- Kasahara, Y.; Sugii, K.; Ohnishi, T.
- Physical Review Letters, Vol. 120, Issue 21
Excitations in the field-induced quantum spin liquid state of α-RuCl3
journal, February 2018
- Banerjee, Arnab; Lampen-Kelley, Paula; Knolle, Johannes
- npj Quantum Materials, Vol. 3, Issue 1
Observation of two types of fractional excitation in the Kitaev honeycomb magnet
journal, May 2018
- Janša, Nejc; Zorko, Andrej; Gomilšek, Matjaž
- Nature Physics, Vol. 14, Issue 8
Physics of the Kitaev Model: Fractionalization, Dynamic Correlations, and Material Connections
journal, March 2018
- Hermanns, M.; Kimchi, I.; Knolle, J.
- Annual Review of Condensed Matter Physics, Vol. 9, Issue 1
Neutron scattering in the proximate quantum spin liquid α-RuCl 3
journal, June 2017
- Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes
- Science, Vol. 356, Issue 6342
Evidence for a spinon Fermi surface in a triangular-lattice quantum-spin-liquid candidate
journal, December 2016
- Shen, Yao; Li, Yao-Dong; Wo, Hongliang
- Nature, Vol. 540, Issue 7634
Enhanced thermal Hall effect in the square-lattice Néel state
journal, October 2019
- Samajdar, Rhine; Scheurer, Mathias S.; Chatterjee, Shubhayu
- Nature Physics, Vol. 15, Issue 12
Sample dependence of half-integer quantized thermal Hall effect in the Kitaev spin-liquid candidate
journal, December 2020
- Yamashita, M.; Gouchi, J.; Uwatoko, Y.
- Physical Review B, Vol. 102, Issue 22
Unusual Phonon Heat Transport in : Strong Spin-Phonon Scattering and Field-Induced Spin Gap
journal, March 2018
- Hentrich, Richard; Wolter, Anja U. B.; Zotos, Xenophon
- Physical Review Letters, Vol. 120, Issue 11
Electromagnon dispersion probed by inelastic X-ray scattering in LiCrO2
journal, November 2016
- Tóth, Sándor; Wehinger, Björn; Rolfs, Katharina
- Nature Communications, Vol. 7, Issue 1
Thermodynamic evidence of fractionalized excitations in
journal, March 2019
- Widmann, S.; Tsurkan, V.; Prishchenko, D. A.
- Physical Review B, Vol. 99, Issue 9
Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid
journal, July 2018
- Kasahara, Y.; Ohnishi, T.; Mizukami, Y.
- Nature, Vol. 559, Issue 7713
Phononic Helical Nodal Lines with Protection in
journal, December 2019
- Zhang, T. T.; Miao, H.; Wang, Q.
- Physical Review Letters, Vol. 123, Issue 24
Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models
journal, February 2019
- Rusnačko, Juraj; Gotfryd, Dorota; Chaloupka, Jiří
- Physical Review B, Vol. 99, Issue 6
Energy Gaps and Kohn Anomalies in Elemental Superconductors
journal, March 2008
- Aynajian, P.; Keller, T.; Boeri, L.
- Science, Vol. 319, Issue 5869
Consideration of thermal Hall effect in undoped cuprates
journal, May 2019
- Han, Jung Hoon; Park, Jin-Hong; Lee, Patrick A.
- Physical Review B, Vol. 99, Issue 20
Phonon renormalization in the Kitaev quantum spin liquid
journal, January 2020
- Metavitsiadis, Alexandros; Brenig, Wolfram
- Physical Review B, Vol. 101, Issue 3
Majorana fermions in the Kitaev quantum spin system α-RuCl3
journal, September 2017
- Do, Seung-Hwan; Park, Sang-Youn; Yoshitake, Junki
- Nature Physics, Vol. 13, Issue 11
Observation of Double Weyl Phonons in Parity-Breaking FeSi
journal, July 2018
- Miao, H.; Zhang, T. T.; Wang, L.
- Physical Review Letters, Vol. 121, Issue 3
Topological quantum chemistry
journal, July 2017
- Bradlyn, Barry; Elcoro, L.; Cano, Jennifer
- Nature, Vol. 547, Issue 7663
Scattering Continuum and Possible Fractionalized Excitations in
journal, April 2015
- Sandilands, Luke J.; Tian, Yao; Plumb, Kemp W.
- Physical Review Letters, Vol. 114, Issue 14
Anomalous Thermal Conductivity and Magnetic Torque Response in the Honeycomb Magnet
journal, May 2017
- Leahy, Ian A.; Pocs, Christopher A.; Siegfried, Peter E.
- Physical Review Letters, Vol. 118, Issue 18
Choreographed entanglement dances: Topological states of quantum matter
journal, February 2019
- Wen, Xiao-Gang
- Science, Vol. 363, Issue 6429
A spin–orbital-entangled quantum liquid on a honeycomb lattice
journal, February 2018
- Kitagawa, K.; Takayama, T.; Matsumoto, Y.
- Nature, Vol. 554, Issue 7692
Chiral phonons in the pseudogap phase of cuprates
journal, July 2020
- Grissonnanche, G.; Thériault, S.; Gourgout, A.
- Nature Physics, Vol. 16, Issue 11
Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet
journal, December 2012
- Han, Tian-Heng; Helton, Joel S.; Chu, Shaoyan
- Nature, Vol. 492, Issue 7429
Phonon dynamics in the Kitaev spin liquid
journal, August 2020
- Ye, Mengxing; Fernandes, Rafael M.; Perkins, Natalia B.
- Physical Review Research, Vol. 2, Issue 3
A practical guide for crystal growth of van der Waals layered materials
journal, August 2020
- May, Andrew F.; Yan, Jiaqiang; McGuire, Michael A.
- Journal of Applied Physics, Vol. 128, Issue 5
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009
- Jackeli, G.; Khaliullin, G.
- Physical Review Letters, Vol. 102, Issue 1
Giant Kohn Anomaly and the Phase Transition in Charge Density Wave
journal, February 2009
- Hoesch, Moritz; Bosak, Alexey; Chernyshov, Dmitry
- Physical Review Letters, Vol. 102, Issue 8
Quantization of the Thermal Hall Conductivity at Small Hall Angles
journal, October 2018
- Ye, Mengxing; Halász, Gábor B.; Savary, Lucile
- Physical Review Letters, Vol. 121, Issue 14
Observation of two types of fractional excitation in the Kitaev honeycomb magnet
journal, May 2018
- Janša, Nejc; Zorko, Andrej; Gomilšek, Matjaž
- Nature Physics, Vol. 14, Issue 8
Thermal Transport in the Kitaev Model
journal, September 2017
- Nasu, Joji; Yoshitake, Junki; Motome, Yukitoshi
- Physical Review Letters, Vol. 119, Issue 12