Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr2IrO4

Porras, J.; Bertinshaw, J.; Liu, H.; Khaliullin, G.; Sung, N. H.; Kim, J. -W.; Francoual, S.; Steffens, P.; Deng, G.; Sala, M. Moretti; Efimenko, A.; Said, A.; Casa, D.; Huang, X.; Gog, T.; Kim, J.; Keimer, B.; Kim, B. J.

doi:10.1103/PhysRevB.99.085125

Title: Pseudospin-lattice coupling in the spin-orbit Mott insulator ${Sr}_{2} {IrO}_{4}$

Abstract

Spin-orbit entangled magnetic dipoles, often referred to as pseudospins, provide a new avenue to explore novel magnetism inconceivable in the weak spin-orbit coupling limit, but the nature of their low-energy interactions remains to be understood. In this paper, we present a comprehensive study of the static magnetism and low-energy pseudospin dynamics in the archetypal spin-orbit Mott insulator Sr₂IrO₄. We find that in order to understand even basic magnetization measurements, a formerly overlooked in-plane anisotropy is fundamental. In addition to magnetometry, we use neutron diffraction, inelastic neutron scattering, and resonant elastic and inelastic x-ray scattering to identify and quantify the interactions that determine the global symmetry of the system and govern the linear responses of pseudospins to external magnetic fields and their low-energy dynamics. We find that a pseudospin-only Hamiltonian is insufficient for an accurate description of the magnetism in Sr₂IrO₄ and that pseudospin-lattice coupling is essential. In conclusion, this finding should be generally applicable to other pseudospin systems with sizable orbital moments sensitive to anisotropic crystalline environment

Authors:

Porras, J. ^[1]; Bertinshaw, J. ^[1]; Liu, H. ^[1]; Khaliullin, G. ^[1]; Sung, N. H. ^[1]; Kim, J. -W. ^[2]; Francoual, S. ^[3]; Steffens, P. ^[4]; Deng, G. ^[5]; Sala, M. Moretti ^[6]; Efimenko, A. ^[7]; Said, A. ^[2]; Casa, D. ^[2]; Huang, X. ^[2]; Gog, T. ^[2]; Kim, J. ^[2]; Keimer, B. ^[1]; Kim, B. J. ^[8]

Max-Planck-Institut für Festkörperforschung, Stuttgart (Germany)
Argonne National Lab. (ANL), Argonne, IL (United States)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Institut Laue-Langevin 6, rue Jules Horowitz (France)
Australian Nuclear Science and Technology Organization, Lucas Height, New South Wales (Australia)
European Synchrotron Radiation Facility (France); Politecnico di Milano, Piazza Leonardo da Vinci, Milano (Italy)
European Synchrotron Radiation Facility (France)
Max-Planck-Institut für Festkörperforschung, Stuttgart (Germany); Pohang University of Science and Technology (South Korea); Institute for Basic Science (South Korea)

Publication Date:: 2019-02-15

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC); Institute for Basic Science

OSTI Identifier:: 1496059

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 99; Journal Issue: 8; 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; 36 MATERIALS SCIENCE

Citation Formats


                    Porras, J., Bertinshaw, J., Liu, H., Khaliullin, G., Sung, N. H., Kim, J. -W., Francoual, S., Steffens, P., Deng, G., Sala, M. Moretti, Efimenko, A., Said, A., Casa, D., Huang, X., Gog, T., Kim, J., Keimer, B., and Kim, B. J. Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr2IrO4.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevB.99.085125.

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                    Porras, J., Bertinshaw, J., Liu, H., Khaliullin, G., Sung, N. H., Kim, J. -W., Francoual, S., Steffens, P., Deng, G., Sala, M. Moretti, Efimenko, A., Said, A., Casa, D., Huang, X., Gog, T., Kim, J., Keimer, B., & Kim, B. J. Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr2IrO4.  United States.  https://doi.org/10.1103/PhysRevB.99.085125

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                    Porras, J., Bertinshaw, J., Liu, H., Khaliullin, G., Sung, N. H., Kim, J. -W., Francoual, S., Steffens, P., Deng, G., Sala, M. Moretti, Efimenko, A., Said, A., Casa, D., Huang, X., Gog, T., Kim, J., Keimer, B., and Kim, B. J. Fri .  
"Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr2IrO4".  United States.  https://doi.org/10.1103/PhysRevB.99.085125.  https://www.osti.gov/servlets/purl/1496059.

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@article{osti_1496059,

  title        = {Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr2IrO4},

  author       = {Porras, J. and Bertinshaw, J. and Liu, H. and Khaliullin, G. and Sung, N. H. and Kim, J. -W. and Francoual, S. and Steffens, P. and Deng, G. and Sala, M. Moretti and Efimenko, A. and Said, A. and Casa, D. and Huang, X. and Gog, T. and Kim, J. and Keimer, B. and Kim, B. J.},

  abstractNote = {Spin-orbit entangled magnetic dipoles, often referred to as pseudospins, provide a new avenue to explore novel magnetism inconceivable in the weak spin-orbit coupling limit, but the nature of their low-energy interactions remains to be understood. In this paper, we present a comprehensive study of the static magnetism and low-energy pseudospin dynamics in the archetypal spin-orbit Mott insulator Sr2IrO4. We find that in order to understand even basic magnetization measurements, a formerly overlooked in-plane anisotropy is fundamental. In addition to magnetometry, we use neutron diffraction, inelastic neutron scattering, and resonant elastic and inelastic x-ray scattering to identify and quantify the interactions that determine the global symmetry of the system and govern the linear responses of pseudospins to external magnetic fields and their low-energy dynamics. We find that a pseudospin-only Hamiltonian is insufficient for an accurate description of the magnetism in Sr2IrO4 and that pseudospin-lattice coupling is essential. In conclusion, this finding should be generally applicable to other pseudospin systems with sizable orbital moments sensitive to anisotropic crystalline environment},

  doi          = {10.1103/PhysRevB.99.085125},

  journal      = {Physical Review B},

  number       = 8,

  volume       = 99,

  place        = {United States},

  year         = {2019},

  month        = {2}

}

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Works referencing / citing this record:

The J _eff = 1/2 Antiferromagnet Sr ₂ IrO ₄ : A Golden Avenue toward New Physics and Functions
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Lu, Chengliang; Liu, Jun‐Ming
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Title: Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr 2 IrO 4

Abstract

Citation Formats

Structural and magnetic studies of Sr 2 IrO 4 journal, April 1994

Effects of an external magnetic field on the gaps and quantum corrections in an ordered Heisenberg antiferromagnet with Dzyaloshinskii-Moriya anisotropy journal, November 2005

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Structural Distortion-Induced Magnetoelastic Locking in Sr 2 IrO 4 Revealed through Nonlinear Optical Harmonic Generation journal, March 2015

Interplay between electron–phonon and Coulomb interactions in cuprates journal, January 2008

High-precision determination of low-energy effective parameters for a two-dimensional Heisenberg quantum antiferromagnet journal, April 2011

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Weak Ferromagnetism and Field-Induced Spin Reorientation in K 2 V 3 O 8 journal, January 2001

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Observation of a d-wave gap in electron-doped Sr2IrO4 journal, October 2015

Linear spin wave theory for single-Q incommensurate magnetic structures journal, March 2015

Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides A 2 IrO 3 journal, July 2010

Large Spin-Wave Energy Gap in the Bilayer Iridate Sr 3 Ir 2 O 7 : Evidence for Enhanced Dipolar Interactions Near the Mott Metal-Insulator Transition journal, October 2012

Magnetic ground state of Sr 2 IrO 4 and implications for second-harmonic generation journal, August 2016

Double Exchange Alone Does Not Explain the Resistivity of La 1 − x Sr x MnO 3 journal, June 1995

Model analysis of magnetic susceptibility of Sr 2 IrO 4 : A two-dimensional J eff = 1 2 Heisenberg system with competing interlayer couplings journal, December 2016

Quartz-based flat-crystal resonant inelastic x-ray scattering spectrometer with sub-10 meV energy resolution journal, January 2018

Higgs mode and its decay in a two-dimensional antiferromagnet journal, March 2017

Persistent Paramagnons Deep in the Metallic Phase of Sr 2 − x La x IrO 4 journal, September 2016

Pseudo-Jahn-Teller Effect and Magnetoelastic Coupling in Spin-Orbit Mott Insulators journal, February 2019

Zigzag Magnetic Order in the Iridium Oxide Na 2 IrO 3 journal, February 2013

Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4 journal, May 2016

Square Lattice Iridates journal, March 2019

Neutron scattering study of correlated phase behavior in Sr 2 IrO 4 journal, April 2013

A high-energy-resolution resonant inelastic X-ray scattering spectrometer at ID20 of the European Synchrotron Radiation Facility journal, February 2018

Orbital Order and Fluctuations in Mott Insulators journal, January 2005

Novel J eff = 1 / 2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4 journal, August 2008

Magnetic and crystal structures of Sr 2 IrO 4 : A neutron diffraction study journal, April 2013

Magnetic critical properties and basal-plane anisotropy of Sr 2 IrO 4 journal, March 2016

High-energy-resolution diced spherical quartz analyzers for resonant inelastic X-ray scattering journal, February 2018

Raman scattering study of vibrational and magnetic excitations in Sr 2 − x La x IrO 4 journal, September 2017

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

Importance of X Y anisotropy in Sr 2 IrO 4 revealed by magnetic critical scattering experiments journal, July 2015

Isotropic and anisotropic regimes of the field-dependent spin dynamics in Sr 2 IrO 4 : Raman scattering studies journal, January 2016

Evidence of quantum dimer excitations in Sr 3 Ir 2 O 7 journal, July 2015

Two-Dimensional Heisenberg Behavior of J eff = 1 / 2 Isospins in the Paramagnetic State of the Spin-Orbital Mott Insulator Sr 2 IrO 4 journal, June 2012

Mechanism of Basal-Plane Antiferromagnetism in the Spin-Orbit Driven Iridate Ba 2 IrO 4 journal, June 2014

Electron-Doped Sr 2 IrO 4 : An Analogue of Hole-Doped Cuprate Superconductors Demonstrated by Scanning Tunneling Microscopy journal, November 2015

Low-energy magnetic excitations in the spin-orbital Mott insulator Sr 2 IrO 4 journal, May 2014

In-plane magnetic anisotropy in strontium iridate S r 2 Ir O 4 journal, October 2017

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

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 journal, May 2015

Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates journal, May 2011

Anisotropic exchange and spin-wave damping in pure and electron-doped Sr 2 IrO 4 journal, August 2017

The J eff = 1/2 Antiferromagnet Sr 2 IrO 4 : A Golden Avenue toward New Physics and Functions journal, October 2019

Giant anisotropic magnetoresistance and nonvolatile memory in canted antiferromagnet Sr2IrO4 journal, May 2019

Isospin-phonon coupling and Fano-interference in spin-orbit Mott insulator Sr 2 IrO 4 journal, April 2019

Symmetry breaking of in-plane anisotropic magnetoresistance with temperature in La-doped S r 2 Ir O 4 films journal, August 2019

First-principles calculation of spin and orbital contributions to magnetically ordered moments in Sr 2 IrO 4 journal, April 2020

Title: Pseudospin-lattice coupling in the spin-orbit Mott insulator ${Sr}_{2} {IrO}_{4}$

Structural and magnetic studies of ${Sr}_{2}$ ${IrO}_{4}$
journal, April 1994

Effects of an external magnetic field on the gaps and quantum corrections in an ordered Heisenberg antiferromagnet with Dzyaloshinskii-Moriya anisotropy
journal, November 2005

Evidence of an odd-parity hidden order in a spin–orbit coupled correlated iridate
journal, October 2015

Magnetic Excitation Spectra of ${Sr}_{2} {IrO}_{4}$ Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors
journal, April 2012

Models and materials for generalized Kitaev magnetism
journal, November 2017

Anisotropic Magnetoresistance in Antiferromagnetic ${Sr}_{2} {IrO}_{4}$
journal, November 2014

Anisotropic spin Hamiltonians due to spin-orbit and Coulomb exchange interactions
journal, October 1995

Excitonic Magnetism in Van Vleck–type $d^{4}$ Mott Insulators
journal, November 2013

Structural Distortion-Induced Magnetoelastic Locking in ${Sr}_{2} {IrO}_{4}$ Revealed through Nonlinear Optical Harmonic Generation
journal, March 2015

Interplay between electron–phonon and Coulomb interactions in cuprates
journal, January 2008

High-precision determination of low-energy effective parameters for a two-dimensional Heisenberg quantum antiferromagnet
journal, April 2011

Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009

Weak Ferromagnetism and Field-Induced Spin Reorientation in $K_{2} V_{3} O_{8}$
journal, January 2001

Fermi arcs in a doped pseudospin-1/2 Heisenberg antiferromagnet
journal, June 2014

Observation of a d-wave gap in electron-doped Sr2IrO4
journal, October 2015

Linear spin wave theory for single-Q incommensurate magnetic structures
journal, March 2015

Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides $A_{2} {IrO}_{3}$
journal, July 2010

Large Spin-Wave Energy Gap in the Bilayer Iridate ${Sr}_{3} {Ir}_{2} O_{7}$ : Evidence for Enhanced Dipolar Interactions Near the Mott Metal-Insulator Transition
journal, October 2012

Magnetic ground state of ${Sr}_{2} {IrO}_{4}$ and implications for second-harmonic generation
journal, August 2016

Double Exchange Alone Does Not Explain the Resistivity of ${La}_{1}_{- x} {Sr}_{x} {MnO}_{3}$
journal, June 1995

Model analysis of magnetic susceptibility of ${Sr}_{2} {IrO}_{4}$ : A two-dimensional $J_{eff} = \frac{1}{2}$ Heisenberg system with competing interlayer couplings
journal, December 2016

Quartz-based flat-crystal resonant inelastic x-ray scattering spectrometer with sub-10 meV energy resolution
journal, January 2018

Higgs mode and its decay in a two-dimensional antiferromagnet
journal, March 2017

Persistent Paramagnons Deep in the Metallic Phase of ${Sr}_{2 - x} {La}_{x} {IrO}_{4}$
journal, September 2016

Pseudo-Jahn-Teller Effect and Magnetoelastic Coupling in Spin-Orbit Mott Insulators
journal, February 2019

Zigzag Magnetic Order in the Iridium Oxide ${Na}_{2} {IrO}_{3}$
journal, February 2013

Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4
journal, May 2016

Square Lattice Iridates
journal, March 2019

Neutron scattering study of correlated phase behavior in Sr $_{2}$ IrO $_{4}$
journal, April 2013

A high-energy-resolution resonant inelastic X-ray scattering spectrometer at ID20 of the European Synchrotron Radiation Facility
journal, February 2018

Orbital Order and Fluctuations in Mott Insulators
journal, January 2005

Novel $J_{eff} = 1 / 2$ Mott State Induced by Relativistic Spin-Orbit Coupling in ${Sr}_{2} {IrO}_{4}$
journal, August 2008

Magnetic and crystal structures of ${Sr}_{2} {IrO}_{4}$ : A neutron diffraction study
journal, April 2013

Magnetic critical properties and basal-plane anisotropy of Sr ₂ IrO ₄
journal, March 2016

High-energy-resolution diced spherical quartz analyzers for resonant inelastic X-ray scattering
journal, February 2018

Raman scattering study of vibrational and magnetic excitations in ${Sr}_{2 - x} {La}_{x} {IrO}_{4}$
journal, September 2017

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

Importance of $X Y$ anisotropy in ${Sr}_{2} {IrO}_{4}$ revealed by magnetic critical scattering experiments
journal, July 2015

Isotropic and anisotropic regimes of the field-dependent spin dynamics in ${Sr}_{2} {IrO}_{4}$ : Raman scattering studies
journal, January 2016

Evidence of quantum dimer excitations in ${Sr}_{3} {Ir}_{2} O_{7}$
journal, July 2015

Two-Dimensional Heisenberg Behavior of $J_{eff} = 1 / 2$ Isospins in the Paramagnetic State of the Spin-Orbital Mott Insulator ${Sr}_{2} {IrO}_{4}$
journal, June 2012

Mechanism of Basal-Plane Antiferromagnetism in the Spin-Orbit Driven Iridate ${Ba}_{2} {IrO}_{4}$
journal, June 2014

Electron-Doped ${Sr}_{2} {IrO}_{4}$ : An Analogue of Hole-Doped Cuprate Superconductors Demonstrated by Scanning Tunneling Microscopy
journal, November 2015

Low-energy magnetic excitations in the spin-orbital Mott insulator ${Sr}_{2} {IrO}_{4}$
journal, May 2014

In-plane magnetic anisotropy in strontium iridate $S r_{2} Ir O_{4}$
journal, October 2017

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

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3
journal, May 2015

Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates
journal, May 2011

Anisotropic exchange and spin-wave damping in pure and electron-doped ${Sr}_{2} {IrO}_{4}$
journal, August 2017

The J _eff = 1/2 Antiferromagnet Sr ₂ IrO ₄ : A Golden Avenue toward New Physics and Functions
journal, October 2019

Giant anisotropic magnetoresistance and nonvolatile memory in canted antiferromagnet Sr2IrO4
journal, May 2019

Isospin-phonon coupling and Fano-interference in spin-orbit Mott insulator Sr ₂ IrO ₄
journal, April 2019

Symmetry breaking of in-plane anisotropic magnetoresistance with temperature in La-doped $S r_{2} Ir O_{4}$ films
journal, August 2019

First-principles calculation of spin and orbital contributions to magnetically ordered moments in ${Sr}_{2} {IrO}_{4}$
journal, April 2020