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Title: Pressure-induced structural dimerization in the hyperhoneycomb iridate β - Li 2 IrO 3 at low temperatures

Abstract

A pressure-induced collapse of magnetic ordering in β-Li 2IrO 3 at P m similar to 1.5-2 GPa has previously been interpreted as evidence for potential emergence of spin liquid states in this hyperhoneycomb iridate, raising prospects for experimental realizations of the Kitaev model. Based on structural data obtained at room temperature, this magnetic transition is believed to originate in small lattice perturbations that preserve crystal symmetry, and related changes in bond-directional anisotropic exchange interactions. In this work, we report on the evolution of the crystal structure of β-Li 2IrO 3 under pressure at low temperatures (T ≤ 50 K) and show that the suppression of magnetism coincides with a change in lattice symmetry involving Ir-Ir dimerization. The critical pressure for dimerization shifts from 4.4(2) GPa at room temperature to similar to 1.5-2 GPa below 50 K. While a direct Fddd → C-2/c transition is observed at room temperature, the low temperature transitions involve new as well as coexisting dimerized phases. Additional investigation of the Ir (L 3/L 2) isotropic branching ratio in x-ray absorption spectra indicates that the previously reported departure of the electronic ground state from a J eff = 1/2 state is closely related to the onset ofmore » dimerized phases. In essence, our results suggest that the predominant mechanism driving the collapse of magnetism in β-Li 2IrO 3 is the pressure-induced formation of Ir 2 dimers in the hyperhoneycomb network. The results further confirm the instability of the J eff = 1/2 moments and related noncollinear spiral magnetic ordering against formation of dimers in the low-temperature phase of compressed β-Li 2IrO 3.« less

Authors:
ORCiD logo [1];  [2];  [3];  [1];  [1];  [4];  [2];  [5];  [6];  [1];  [7];  [7];  [3]
  1. Univ. College London, Bloomsbury (United Kingdom)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. of Illinois, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Ehime Univ., Matsuyama (Japan); Tokyo Institute of Technology (Japan)
  6. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  7. Max Planck Inst. for Solid State Research, Stuttgart (Germany); Univ. of Tokyo (Japan)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1574949
Alternate Identifier(s):
OSTI ID: 1558155
Grant/Contract Number:  
AC02-06CH11357; AC-02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 100; Journal Issue: 6; 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

Veiga, L. S. I., Glazyrin, K., Fabbris, G., Dashwood, C. D., Vale, J. G., Park, H., Etter, M., Irifune, T., Pascarelli, S., McMorrow, D. F., Takayama, T., Takagi, H., and Haskel, D. Pressure-induced structural dimerization in the hyperhoneycomb iridate β-Li2IrO3 at low temperatures. United States: N. p., 2019. Web. doi:10.1103/PhysRevB.100.064104.
Veiga, L. S. I., Glazyrin, K., Fabbris, G., Dashwood, C. D., Vale, J. G., Park, H., Etter, M., Irifune, T., Pascarelli, S., McMorrow, D. F., Takayama, T., Takagi, H., & Haskel, D. Pressure-induced structural dimerization in the hyperhoneycomb iridate β-Li2IrO3 at low temperatures. United States. doi:10.1103/PhysRevB.100.064104.
Veiga, L. S. I., Glazyrin, K., Fabbris, G., Dashwood, C. D., Vale, J. G., Park, H., Etter, M., Irifune, T., Pascarelli, S., McMorrow, D. F., Takayama, T., Takagi, H., and Haskel, D. Wed . "Pressure-induced structural dimerization in the hyperhoneycomb iridate β-Li2IrO3 at low temperatures". United States. doi:10.1103/PhysRevB.100.064104. https://www.osti.gov/servlets/purl/1574949.
@article{osti_1574949,
title = {Pressure-induced structural dimerization in the hyperhoneycomb iridate β-Li2IrO3 at low temperatures},
author = {Veiga, L. S. I. and Glazyrin, K. and Fabbris, G. and Dashwood, C. D. and Vale, J. G. and Park, H. and Etter, M. and Irifune, T. and Pascarelli, S. and McMorrow, D. F. and Takayama, T. and Takagi, H. and Haskel, D.},
abstractNote = {A pressure-induced collapse of magnetic ordering in β-Li2IrO3 at Pm similar to 1.5-2 GPa has previously been interpreted as evidence for potential emergence of spin liquid states in this hyperhoneycomb iridate, raising prospects for experimental realizations of the Kitaev model. Based on structural data obtained at room temperature, this magnetic transition is believed to originate in small lattice perturbations that preserve crystal symmetry, and related changes in bond-directional anisotropic exchange interactions. In this work, we report on the evolution of the crystal structure of β-Li2IrO3 under pressure at low temperatures (T ≤ 50 K) and show that the suppression of magnetism coincides with a change in lattice symmetry involving Ir-Ir dimerization. The critical pressure for dimerization shifts from 4.4(2) GPa at room temperature to similar to 1.5-2 GPa below 50 K. While a direct Fddd → C-2/c transition is observed at room temperature, the low temperature transitions involve new as well as coexisting dimerized phases. Additional investigation of the Ir (L3/L2) isotropic branching ratio in x-ray absorption spectra indicates that the previously reported departure of the electronic ground state from a Jeff = 1/2 state is closely related to the onset of dimerized phases. In essence, our results suggest that the predominant mechanism driving the collapse of magnetism in β-Li2IrO3 is the pressure-induced formation of Ir2 dimers in the hyperhoneycomb network. The results further confirm the instability of the Jeff = 1/2 moments and related noncollinear spiral magnetic ordering against formation of dimers in the low-temperature phase of compressed β-Li2IrO3.},
doi = {10.1103/PhysRevB.100.064104},
journal = {Physical Review B},
issn = {2469-9950},
number = 6,
volume = 100,
place = {United States},
year = {2019},
month = {8}
}

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Works referenced in this record:

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Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in γ Li 2 IrO 3
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Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of α RuCl 3
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Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
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Hyperhoneycomb Iridate β Li 2 IrO 3 as a Platform for Kitaev Magnetism
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Orbital Magnetism and Spin-Orbit Effects in the Electronic Structure of BaIrO 3
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Antiferromagnetic Mott insulating state in single crystals of the honeycomb lattice material Na 2 IrO 3
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Correlated states in β-Li2IrO3 driven by applied magnetic fields
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Bond ordering and phase transitions in Na 2 IrO 3 under high pressure
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Phase diagram of α RuCl 3 in an in-plane magnetic field
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Pressure-induced collapse of the spin-orbital Mott state in the hyperhoneycomb iridate β Li 2 IrO 3
journal, March 2019


Finite Elastic Strain of Cubic Crystals
journal, June 1947


Effect of isoelectronic doping on the honeycomb-lattice iridate A 2 IrO 3
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Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: α Li 2 IrO 3 under pressure
journal, January 2018


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A spin–orbital-entangled quantum liquid on a honeycomb lattice
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Three-dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite- D approximation
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Raman Scattering Signatures of Kitaev Spin Liquids in A 2 IrO 3 Iridates with A = Na or Li
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Pressure Tuning of the Spin-Orbit Coupled Ground State in Sr 2 IrO 4
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Monoclinic crystal structure of α RuCl 3 and the zigzag antiferromagnetic ground state
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High-temperature magnetostructural transition in van der Waals-layered α MoCl 3
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Topological and magnetic phases of interacting electrons in the pyrochlore iridates
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Unusual Phonon Heat Transport in α RuCl 3 : Strong Spin-Phonon Scattering and Field-Induced Spin Gap
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Resonant x-ray scattering reveals possible disappearance of magnetic order under hydrostatic pressure in the Kitaev candidate γ Li 2 IrO 3
journal, July 2017


Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates A 2 IrO 3
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Spin Waves and Revised Crystal Structure of Honeycomb Iridate Na 2 IrO 3
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The vicinity of hyper-honeycomb β-Li2IrO3 to a three-dimensional Kitaev spin liquid state
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Hydrostatic limits of 11 pressure transmitting media
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Long-range magnetic ordering in Na 2 IrO 3
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    Works referencing / citing this record:

    Ultrahard polycrystalline diamond from graphite
    journal, February 2003

    • Irifune, Tetsuo; Kurio, Ayako; Sakamoto, Shizue
    • Nature, Vol. 421, Issue 6923
    • DOI: 10.1038/421599b

    Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in γ Li 2 IrO 3
    journal, November 2014


    Models and materials for generalized Kitaev magnetism
    journal, November 2017

    • Winter, Stephen M.; Tsirlin, Alexander A.; Daghofer, Maria
    • Journal of Physics: Condensed Matter, Vol. 29, Issue 49
    • DOI: 10.1088/1361-648x/aa8cf5

    Revealing frustrated local moment model for pressurized hyperhoneycomb iridate: Paving the way toward a quantum spin liquid
    journal, December 2016


    Cu 2 IrO 3 : A New Magnetically Frustrated Honeycomb Iridate
    journal, October 2017

    • Abramchuk, Mykola; Ozsoy-Keskinbora, Cigdem; Krizan, Jason W.
    • Journal of the American Chemical Society, Vol. 139, Issue 43
    • DOI: 10.1021/jacs.7b06911

    Pressure Tuning of the Spin-Orbit Coupled Ground State in Sr 2 IrO 4
    journal, July 2012


    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
    • DOI: 10.1038/nmat4604

    The vicinity of hyper-honeycomb β-Li2IrO3 to a three-dimensional Kitaev spin liquid state
    journal, July 2016

    • Katukuri, Vamshi M.; Yadav, Ravi; Hozoi, Liviu
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep29585

    Two-dimensional detector software: From real detector to idealised image or two-theta scan
    journal, January 1996

    • Hammersley, A. P.; Svensson, S. O.; Hanfland, M.
    • High Pressure Research, Vol. 14, Issue 4-6, p. 235-248
    • DOI: 10.1080/08957959608201408

    Predominance of the Kitaev interaction in a three-dimensional honeycomb iridate: From ab initio to spin model
    journal, December 2015


    Breakdown of Magnetic Order in the Pressurized Kitaev Iridate β Li 2 IrO 3
    journal, June 2018


    Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
    journal, March 2016


    Spin Waves and Revised Crystal Structure of Honeycomb Iridate Na 2 IrO 3
    journal, March 2012


    Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates A 2 IrO 3
    journal, March 2012


    Unusual Phonon Heat Transport in α RuCl 3 : Strong Spin-Phonon Scattering and Field-Induced Spin Gap
    journal, March 2018


    Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
    journal, January 2009


    Finite Elastic Strain of Cubic Crystals
    journal, June 1947


    Pressure-induced structural dimerization in the hyperhoneycomb iridate $β−Li_{2}IrO_{3}$ at low temperatures
    text, January 2019

    • Veiga, L. S. I.; Glazyrin, K.; Fabbris, G.
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-03160

    Pressure tuning of bond-directional exchange interactions and magnetic frustration in the hyperhoneycomb iridate β Li 2 IrO 3
    journal, October 2017


    Hydrostatic limits of 11 pressure transmitting media
    journal, March 2009

    • Klotz, S.; Chervin, J-C.; Munsch, P.
    • Journal of Physics D: Applied Physics, Vol. 42, Issue 7, Article No. 075413
    • DOI: 10.1088/0022-3727/42/7/075413

    Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet α RuCl 3
    journal, June 2018


    Pressure-induced collapse of the spin-orbital Mott state in the hyperhoneycomb iridate β Li 2 IrO 3
    journal, March 2019


    Bond ordering and phase transitions in Na 2 IrO 3 under high pressure
    journal, September 2018


    Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate
    journal, June 2014

    • Modic, K. A.; Smidt, Tess E.; Kimchi, Itamar
    • Nature Communications, Vol. 5, Issue 1
    • DOI: 10.1038/ncomms5203

    Glitch-free X-ray absorption spectrum under high pressure obtained using nano-polycrystalline diamond anvils
    journal, July 2012

    • Ishimatsu, Naoki; Matsumoto, Ken; Maruyama, Hiroshi
    • Journal of Synchrotron Radiation, Vol. 19, Issue 5
    • DOI: 10.1107/s0909049512026088

    Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: α Li 2 IrO 3 under pressure
    journal, January 2018


    Antiferromagnetic Mott insulating state in single crystals of the honeycomb lattice material Na 2 IrO 3
    journal, August 2010


    Orbital Magnetism and Spin-Orbit Effects in the Electronic Structure of BaIrO 3
    journal, November 2010


    Effect of isoelectronic doping on the honeycomb-lattice iridate A 2 IrO 3
    journal, June 2014


    Hyperhoneycomb Iridate β Li 2 IrO 3 as a Platform for Kitaev Magnetism
    journal, February 2015


    EXPGUI , a graphical user interface for GSAS
    journal, April 2001


    Long-range magnetic ordering in Na 2 IrO 3
    journal, June 2011


    Raman Scattering Signatures of Kitaev Spin Liquids in A 2 IrO 3 Iridates with A = Na or Li
    journal, October 2014


    Low-temperature crystal and magnetic structure of α RuCl 3
    journal, April 2016


    Monoclinic crystal structure of α RuCl 3 and the zigzag antiferromagnetic ground state
    journal, December 2015


    α RuCl 3 : A spin-orbit assisted Mott insulator on a honeycomb lattice
    journal, July 2014


    Correlated states in β-Li2IrO3 driven by applied magnetic fields
    journal, October 2017


    Anyons in an exactly solved model and beyond
    journal, January 2006


    Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales
    journal, June 2016


    Electronic structure, local magnetism, and spin-orbit effects of Ir(IV)-, Ir(V)-, and Ir(VI)-based compounds
    journal, June 2015


    Incommensurate counterrotating magnetic order stabilized by Kitaev interactions in the layered honeycomb α Li 2 IrO 3
    journal, May 2016


    OLEX2 : a complete structure solution, refinement and analysis program
    journal, January 2009

    • Dolomanov, Oleg V.; Bourhis, Luc J.; Gildea, Richard J.
    • Journal of Applied Crystallography, Vol. 42, Issue 2
    • DOI: 10.1107/s0021889808042726

    High-temperature magnetostructural transition in van der Waals-layered α MoCl 3
    journal, November 2017


    Generalized Gradient Approximation Made Simple
    journal, October 1996

    • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
    • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
    • DOI: 10.1103/physrevlett.77.3865

    New-Type Phase Transition of Li 2 RuO 3 with Honeycomb Structure
    journal, March 2007

    • Miura, Yoko; Yasui, Yukio; Sato, Masatoshi
    • Journal of the Physical Society of Japan, Vol. 76, Issue 3
    • DOI: 10.1143/jpsj.76.033705

    Robust spin correlations at high magnetic fields in the harmonic honeycomb iridates
    journal, August 2017


    Gapless Spin Excitations in the Field-Induced Quantum Spin Liquid Phase of α RuCl 3
    journal, December 2017


    Spin-orbit coupling in iridium-based 5 d compounds probed by x-ray absorption spectroscopy
    journal, November 2012


    Three-dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite- D approximation
    journal, November 2014


    Phase diagram of α RuCl 3 in an in-plane magnetic field
    journal, May 2017


    Spin liquids in frustrated magnets
    journal, March 2010


    Resonant x-ray scattering reveals possible disappearance of magnetic order under hydrostatic pressure in the Kitaev candidate γ Li 2 IrO 3
    journal, July 2017


    Topological and magnetic phases of interacting electrons in the pyrochlore iridates
    journal, January 2012


    From ultrasoft pseudopotentials to the projector augmented-wave method
    journal, January 1999


    A spin–orbital-entangled quantum liquid on a honeycomb lattice
    journal, February 2018

    • Kitagawa, K.; Takayama, T.; Matsumoto, Y.
    • Nature, Vol. 554, Issue 7692
    • DOI: 10.1038/nature25482

    Local Probe for Spin-Orbit Interaction
    journal, May 1988


    Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
    journal, October 1996