Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet
Abstract
Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material α-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p ~ 0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin-liquid phase in α-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.
- Authors:
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); German Research Foundation (DFG); European Commission (EC); Gordon and Betty Moore Foundation
- OSTI Identifier:
- 1454369
- Alternate Identifier(s):
- OSTI ID: 1761764
- Grant/Contract Number:
- AC05-00OR22725; SFB 1143; WO 1532/3-2; 796048; GBMF4416
- Resource Type:
- Published Article
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Name: Physical Review. B Journal Volume: 97 Journal Issue: 24; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Bastien, G., Garbarino, G., Yadav, R., Martinez-Casado, F. J., Beltrán Rodríguez, R., Stahl, Q., Kusch, M., Limandri, S. P., Ray, R., Lampen-Kelley, P., Mandrus, D. G., Nagler, S. E., Roslova, M., Isaeva, A., Doert, T., Hozoi, L., Wolter, A. U. B., Büchner, B., Geck, J., and van den Brink, J. Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α − RuCl 3. United States: N. p., 2018.
Web. doi:10.1103/PhysRevB.97.241108.
Bastien, G., Garbarino, G., Yadav, R., Martinez-Casado, F. J., Beltrán Rodríguez, R., Stahl, Q., Kusch, M., Limandri, S. P., Ray, R., Lampen-Kelley, P., Mandrus, D. G., Nagler, S. E., Roslova, M., Isaeva, A., Doert, T., Hozoi, L., Wolter, A. U. B., Büchner, B., Geck, J., & van den Brink, J. Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α − RuCl 3. United States. https://doi.org/10.1103/PhysRevB.97.241108
Bastien, G., Garbarino, G., Yadav, R., Martinez-Casado, F. J., Beltrán Rodríguez, R., Stahl, Q., Kusch, M., Limandri, S. P., Ray, R., Lampen-Kelley, P., Mandrus, D. G., Nagler, S. E., Roslova, M., Isaeva, A., Doert, T., Hozoi, L., Wolter, A. U. B., Büchner, B., Geck, J., and van den Brink, J. Fri .
"Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α − RuCl 3". United States. https://doi.org/10.1103/PhysRevB.97.241108.
@article{osti_1454369,
title = {Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α − RuCl 3},
author = {Bastien, G. and Garbarino, G. and Yadav, R. and Martinez-Casado, F. J. and Beltrán Rodríguez, R. and Stahl, Q. and Kusch, M. and Limandri, S. P. and Ray, R. and Lampen-Kelley, P. and Mandrus, D. G. and Nagler, S. E. and Roslova, M. and Isaeva, A. and Doert, T. and Hozoi, L. and Wolter, A. U. B. and Büchner, B. and Geck, J. and van den Brink, J.},
abstractNote = {Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material α-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p ~ 0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin-liquid phase in α-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.},
doi = {10.1103/PhysRevB.97.241108},
journal = {Physical Review. B},
number = 24,
volume = 97,
place = {United States},
year = {Fri Jun 15 00:00:00 EDT 2018},
month = {Fri Jun 15 00:00:00 EDT 2018}
}
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https://doi.org/10.1103/PhysRevB.97.241108
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Works referenced in this record:
Field-induced quantum criticality in the Kitaev system
journal, July 2017
- Wolter, A. U. B.; Corredor, L. T.; Janssen, L.
- Physical Review B, Vol. 96, Issue 4
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
Anyons in an exactly solved model and beyond
journal, January 2006
- Kitaev, Alexei
- Annals of Physics, Vol. 321, Issue 1
High-temperature magnetostructural transition in van der Waals-layered
journal, November 2017
- McGuire, Michael A.; Yan, Jiaqiang; Lampen-Kelley, Paula
- Physical Review Materials, Vol. 1, Issue 6
High-pressure magnetization and NMR studies of
journal, November 2017
- Cui, Y.; Zheng, J.; Ran, K.
- Physical Review B, Vol. 96, Issue 20
WinGX suite for small-molecule single-crystal crystallography
journal, August 1999
- Farrugia, Louis J.
- Journal of Applied Crystallography, Vol. 32, Issue 4
Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales
journal, June 2016
- Winter, Stephen M.; Li, Ying; Jeschke, Harald O.
- Physical Review B, Vol. 93, Issue 21
A short history of SHELX
journal, December 2007
- Sheldrick, George M.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 64, Issue 1, p. 112-122
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
Molecular Electronic-Structure Theory
book, August 2000
- Helgaker, Trygve; Jørgensen, Poul; Olsen, Jeppe
Phase diagram of in an in-plane magnetic field
journal, May 2017
- Sears, J. A.; Zhao, Y.; Xu, Z.
- Physical Review B, Vol. 95, Issue 18
Molpro: a general-purpose quantum chemistry program package: Molpro
journal, July 2011
- Werner, Hans-Joachim; Knowles, Peter J.; Knizia, Gerald
- Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2
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
About Trihalides with TiI3 Chain Structure: Proof of Pair Forming of Cations in ?-RuCl3 and RuBr3 by Temperature Dependent Single Crystal X-ray Analyses
journal, November 2004
- Hillebrecht, H.; Ludwig, Th.; Thiele, G.
- Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 630, Issue 13-14
Neue Untersuchungen �ber die Chloride des Molybd�ns
journal, September 1967
- Sch�fer, H.; Schnering, H. -G. V.; Tillack, J.
- Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 353, Issue 5-6
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
Energy-consistent relativistic pseudopotentials and correlation consistent basis sets for the 4d elements Y–Pd
journal, March 2007
- Peterson, Kirk A.; Figgen, Detlev; Dolg, Michael
- The Journal of Chemical Physics, Vol. 126, Issue 12
Evidence for a Field-Induced Quantum Spin Liquid in -
journal, July 2017
- Baek, S. -H.; Do, S. -H.; Choi, K. -Y.
- Physical Review Letters, Vol. 119, Issue 3
Probing Beyond Magnetic Order: Effects of Temperature and Magnetic Field
journal, February 2018
- Winter, Stephen M.; Riedl, Kira; Kaib, David
- Physical Review Letters, Vol. 120, Issue 7
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
Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: under pressure
journal, January 2018
- Hermann, V.; Altmeyer, M.; Ebad-Allah, J.
- Physical Review B, Vol. 97, Issue 2
Accurate crystal fields for embedded cluster calculations
journal, September 2000
- Klintenberg, M.; Derenzo, S. E.; Weber, M. J.
- Computer Physics Communications, Vol. 131, Issue 1-2
Anisotropic magnetism in the honeycomb system: Susceptibility, specific heat, and zero-field NMR
journal, May 2015
- Majumder, M.; Schmidt, M.; Rosner, H.
- Physical Review B, Vol. 91, Issue 18
Dimer phases in quantum antiferromagnets with orbital degeneracy
journal, October 2007
- Jackeli, G.; Ivanov, D. A.
- Physical Review B, Vol. 76, Issue 13
Ultralow-Temperature Thermal Conductivity of the Kitaev Honeycomb Magnet across the Field-Induced Phase Transition
journal, February 2018
- Yu, Y. J.; Xu, Y.; Ran, K. J.
- Physical Review Letters, Vol. 120, Issue 6
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
Gaussian basis sets for use in correlated molecular calculations. III. The atoms aluminum through argon
journal, January 1993
- Woon, David E.; Dunning, Thom H.
- The Journal of Chemical Physics, Vol. 98, Issue 2
Antiferromagnetic Resonance and Terahertz Continuum in
journal, November 2017
- Little, A.; Wu, Liang; Lampen-Kelley, P.
- Physical Review Letters, Vol. 119, Issue 22
Magnetization processes of zigzag states on the honeycomb lattice: Identifying spin models for and
journal, August 2017
- Janssen, Lukas; Andrade, Eric C.; Vojta, Matthias
- Physical Review B, Vol. 96, Issue 6
Orbital reconstruction in nonpolar tetravalent transition-metal oxide layers
journal, June 2015
- Bogdanov, Nikolay A.; Katukuri, Vamshi M.; Romhányi, Judit
- Nature Communications, Vol. 6, Issue 1
Magnetic Excitations and Continuum of a Possibly Field-Induced Quantum Spin Liquid in
journal, November 2017
- Wang, Zhe; Reschke, S.; Hüvonen, D.
- Physical Review Letters, Vol. 119, Issue 22
Density matrix averaged atomic natural orbital (ANO) basis sets for correlated molecular wave functions: IV. Medium size basis sets for the atoms H-Kr
journal, January 1995
- Pierloot, Kristine; Dumez, Birgit; Widmark, Per-Olof
- Theoretica Chimica Acta, Vol. 90, Issue 2-3
Spin-orbit matrix elements for internally contracted multireference configuration interaction wavefunctions
journal, November 2000
- Berning, Andreas; Schweizer, Marcus; Werner, Hans-Joachim
- Molecular Physics, Vol. 98, Issue 21
Dynamics of fractionalization in quantum spin liquids
journal, September 2015
- Knolle, J.; Kovrizhin, D. L.; Chalker, J. T.
- Physical Review B, Vol. 92, Issue 11
Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3
journal, November 2016
- Yadav, Ravi; Bogdanov, Nikolay A.; Katukuri, Vamshi M.
- Scientific Reports, Vol. 6, Issue 1
Covalent bonds against magnetism in transition metal compounds
journal, September 2016
- Streltsov, Sergey V.; Khomskii, Daniel I.
- Proceedings of the National Academy of Sciences, Vol. 113, Issue 38
Crystal structure and magnetism in : An ab initio study
journal, April 2016
- Kim, Heung-Sik; Kee, Hae-Young
- Physical Review B, Vol. 93, Issue 15
Classical Dimers and Dimerized Superstructure in an Orbitally Degenerate Honeycomb Antiferromagnet
journal, April 2008
- Jackeli, G.; Khomskii, D. I.
- Physical Review Letters, Vol. 100, Issue 14
Miniature ceramic-anvil high-pressure cell for magnetic measurements in a commercial superconducting quantum interference device magnetometer
journal, May 2011
- Tateiwa, Naoyuki; Haga, Yoshinori; Fisk, Zachary
- Review of Scientific Instruments, Vol. 82, Issue 5
Low-temperature crystal and magnetic structure of
journal, April 2016
- Cao, H. B.; Banerjee, A.; Yan, J. -Q.
- Physical Review B, Vol. 93, Issue 13