Magnetic ground state of Sr2IrO4 and implications for second-harmonic generation

Di Matteo, S.; Norman, M. R.

doi:10.1103/PhysRevB.94.075148

Title: Magnetic ground state of ${Sr}_{2} {IrO}_{4}$ and implications for second-harmonic generation

Abstract

The currently accepted magnetic ground state of Sr₂IrO₄ (the -++- state) preserves inversion symmetry. This is at odds, though, with recent experiments that indicate a magnetoelectric ground state, leading to the speculation that orbital currents or more exotic magnetic multipoles might exist in this material. In this paper, we analyze various magnetic configurations and demonstrate that two of them, the magnetoelectric -+-+ state and the nonmagnetoelectric ++++ state, can explain these recent second-harmonic generation (SHG) experiments, obviating the need to invoke orbital currents. The SHG-probed magnetic order parameter has the symmetry of a parity-breaking multipole in the -+-+ state and of a parity-preserving multipole in the ++++ state. We speculate that either might have been created by the laser pump used in the experiments. An alternative is that the observed magnetic SHG signal is a surface effect. Finally, we suggest experiments that could be performed to test these various possibilities and also address the important issue of the suppression of the RXS intensity at the L₂ edge.

Authors:

Di Matteo, S. ^[1]; Norman, M. R. ^[2]

Univ. of Rennes 1 (France). Inst. of Physics of Rennes. Dept. of Materials and Nanoscience
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

Publication Date:: Wed Aug 24 00:00:00 EDT 2016

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Org.:: Univ. of Rennes 1 (France)

OSTI Identifier:: 1352667

Alternate Identifier(s):: OSTI ID: 1305442

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 94; Journal Issue: 7; 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; magnetism; ab initio calculations; resonant inelastic x-ray scattering; x-ray absorption spectroscopy

Citation Formats


                    Di Matteo, S., and Norman, M. R. Magnetic ground state of Sr2IrO4 and implications for second-harmonic generation.  United States: N. p., 2016. 
Web.  doi:10.1103/PhysRevB.94.075148.

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                    Di Matteo, S., & Norman, M. R. Magnetic ground state of Sr2IrO4 and implications for second-harmonic generation.  United States.  https://doi.org/10.1103/PhysRevB.94.075148

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                    Di Matteo, S., and Norman, M. R. Wed .  
"Magnetic ground state of Sr2IrO4 and implications for second-harmonic generation".  United States.  https://doi.org/10.1103/PhysRevB.94.075148.  https://www.osti.gov/servlets/purl/1352667.

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@article{osti_1352667,

  title        = {Magnetic ground state of Sr2IrO4 and implications for second-harmonic generation},

  author       = {Di Matteo, S. and Norman, M. R.},

  abstractNote = {The currently accepted magnetic ground state of Sr2IrO4 (the -++- state) preserves inversion symmetry. This is at odds, though, with recent experiments that indicate a magnetoelectric ground state, leading to the speculation that orbital currents or more exotic magnetic multipoles might exist in this material. In this paper, we analyze various magnetic configurations and demonstrate that two of them, the magnetoelectric -+-+ state and the nonmagnetoelectric ++++ state, can explain these recent second-harmonic generation (SHG) experiments, obviating the need to invoke orbital currents. The SHG-probed magnetic order parameter has the symmetry of a parity-breaking multipole in the -+-+ state and of a parity-preserving multipole in the ++++ state. We speculate that either might have been created by the laser pump used in the experiments. An alternative is that the observed magnetic SHG signal is a surface effect. Finally, we suggest experiments that could be performed to test these various possibilities and also address the important issue of the suppression of the RXS intensity at the L2 edge.},

  doi          = {10.1103/PhysRevB.94.075148},

  journal      = {Physical Review B},

  number       = 7,

  volume       = 94,

  place        = {United States},

  year         = {Wed Aug 24 00:00:00 EDT 2016},

  month        = {Wed Aug 24 00:00:00 EDT 2016}

}

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Sr ₅ Os ₃ O ₁₃ : a mixed valence osmium( v , vi ) layered perovskite variant exhibiting temperature dependent charge distribution
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Title: Magnetic ground state of Sr 2 IrO 4 and implications for second-harmonic generation

Abstract

Citation Formats

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

Disentangling multipole resonances through a full x-ray polarization analysis journal, November 2007

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

Natural widths of atomic K and L levels, K α X‐ray lines and several K L L Auger lines journal, April 1979

Structure symmetry determination and magnetic evolution in Sr 2 Ir 1 − x Rh x O 4 journal, November 2015

Impulsive Generation of Coherent Magnons by Linearly Polarized Light in the Easy-Plane Antiferromagnet FeBO 3 journal, October 2007

Resonant optical control of the structural distortions that drive ultrafast demagnetization in Cr 2 O 3 journal, July 2016

Invisible structures in the X-ray absorption spectra of actinides journal, June 2014

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

Sensitivity to Actinide Doping of Uranium Compounds by Resonant Inelastic X-ray Scattering at Uranium L 3 Edge journal, August 2015

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

X-ray natural circular dichroism journal, September 2000

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

Evolution of competing magnetic order in the J eff = 1 / 2 insulating state of Sr 2 Ir 1 − x Ru x O 4 journal, October 2015

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

Magnetic structural change of Sr 2 IrO 4 upon Mn doping journal, December 2012

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

Coherent ultrafast magnetism induced by femtosecond laser pulses journal, May 2009

Magnetization-induced-second-harmonic generation from surfaces and interfaces journal, January 2005

Role of resonant inelastic X-ray scattering in high-resolution core-level spectroscopy of actinide materials journal, June 2014

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

Magnetic symmetries in neutron and resonant x-ray Bragg diffraction patterns of four iridium oxides journal, November 2012

Self-consistent aspects of x-ray absorption calculations journal, August 2009

Magnetochiral dichroism in Cr 2 O 3 journal, December 2002

Observation of a metal-to-insulator transition with both Mott-Hubbard and Slater characteristics in Sr 2 IrO 4 from time-resolved photocarrier dynamics journal, July 2012

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

Resonant X-Ray Scattering and the j eff = 1 / 2 Electronic Ground State in Iridate Perovskites journal, January 2014

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

Experimental evidence of anapolar moments in the antiferromagnetic insulating phase of V 2 O 3 obtained from x-ray resonant Bragg diffraction journal, February 2010

Crystal field splitting in Sr n + 1 Ir n O 3 n + 1 ( n = 1 , 2 ) iridates probed by x-ray Raman spectroscopy journal, August 2014

Interference of second harmonics due to electric and magnetic dipoles in antiferromagnetic Cr 2 O 3 journal, October 1998

Optical dichroism: E1–M1 integral relations journal, February 2006

Orbital-dependent polaron formation in the relativistic Mott insulator Sr 2 IrO 4 journal, July 2014

Resonant x-ray diffraction: multipole interpretation journal, March 2012

Resonant x-ray scattering as a probe of toroidal moments in centrosymmetric systems journal, October 2004

Anisotropic magnetization-induced second harmonic generation in Fe/Au superlattices journal, October 2001

Non-Fermi-liquid states and pairing instability of a general model of copper oxide metals journal, June 1997

Second-harmonic generation as a tool for studying electronic and magnetic structures of crystals: review journal, January 2005

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

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

Femtosecond switching of magnetism via strongly correlated spin–charge quantum excitations journal, April 2013

Symmetry considerations for detection of time-reversal breaking phases in cuprates by x-ray diffraction and absorption journal, April 2003

Robustness of Basal-Plane Antiferromagnetic Order and the J eff = 1 / 2 State in Single-Layer Iridate Spin-Orbit Mott Insulators journal, March 2013

Giant magnetoelectric effect in the J eff = 1 2 Mott insulator Sr 2 IrO 4 journal, October 2009

Dilute magnetism and spin-orbital percolation effects in Sr 2 Ir 1 − x Rh x O 4 journal, February 2014

Locking of iridium magnetic moments to the correlated rotation of oxygen octahedra in Sr 2 IrO 4 revealed by x-ray resonant scattering journal, September 2013

Electronic structures of layered perovskite Sr 2 M O 4 ( M = Ru , Rh, and Ir) journal, September 2006

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

Interplay of many-body and single-particle interactions in iridates and rhodates journal, January 2014

X-Ray Magnetochiral Dichroism: A New Spectroscopic Probe of Parity Nonconserving Magnetic Solids journal, May 2002

Observation of a $d$-wave gap in electron-doped Sr$_2$IrO$_4$ text, January 2015

Disentangling multipole resonances through a full x-ray polarization analysis text, January 2006

Direct experimental observation of the molecular J eff = 3/2 ground state in the lacunar spinel GaTa4Se8 journal, October 2017

Sr 5 Os 3 O 13 : a mixed valence osmium( v , vi ) layered perovskite variant exhibiting temperature dependent charge distribution journal, January 2018

Magnetic hexadecapole order and magnetopiezoelectric metal state in Ba 1 − x K x Mn 2 As 2 journal, August 2017

Title: Magnetic ground state of ${Sr}_{2} {IrO}_{4}$ and implications for second-harmonic generation

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

Disentangling multipole resonances through a full x-ray polarization analysis
journal, November 2007

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

Natural widths of atomic K and L levels, K α X‐ray lines and several K L L Auger lines
journal, April 1979

Structure symmetry determination and magnetic evolution in ${Sr}_{2} {Ir}_{1 - x} {Rh}_{x} O_{4}$
journal, November 2015

Impulsive Generation of Coherent Magnons by Linearly Polarized Light in the Easy-Plane Antiferromagnet ${FeBO}_{3}$
journal, October 2007

Resonant optical control of the structural distortions that drive ultrafast demagnetization in ${Cr}_{2} O_{3}$
journal, July 2016

Invisible structures in the X-ray absorption spectra of actinides
journal, June 2014

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

Sensitivity to Actinide Doping of Uranium Compounds by Resonant Inelastic X-ray Scattering at Uranium L ₃ Edge
journal, August 2015

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

X-ray natural circular dichroism
journal, September 2000

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

Evolution of competing magnetic order in the $J_{eff} = 1 / 2$ insulating state of ${Sr}_{2} {Ir}_{1 - x} {Ru}_{x} O_{4}$
journal, October 2015

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

Magnetic structural change of Sr $_{2}$ IrO $_{4}$ upon Mn doping
journal, December 2012

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

Coherent ultrafast magnetism induced by femtosecond laser pulses
journal, May 2009

Magnetization-induced-second-harmonic generation from surfaces and interfaces
journal, January 2005

Role of resonant inelastic X-ray scattering in high-resolution core-level spectroscopy of actinide materials
journal, June 2014

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

Magnetic symmetries in neutron and resonant x-ray Bragg diffraction patterns of four iridium oxides
journal, November 2012

Self-consistent aspects of x-ray absorption calculations
journal, August 2009

Magnetochiral dichroism in ${Cr}_{2} O_{3}$
journal, December 2002

Observation of a metal-to-insulator transition with both Mott-Hubbard and Slater characteristics in Sr $_{2}$ IrO $_{4}$ from time-resolved photocarrier dynamics
journal, July 2012

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

Resonant X-Ray Scattering and the $j_{eff} = 1 / 2$ Electronic Ground State in Iridate Perovskites
journal, January 2014

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

Experimental evidence of anapolar moments in the antiferromagnetic insulating phase of $V_{2} O_{3}$ obtained from x-ray resonant Bragg diffraction
journal, February 2010

Crystal field splitting in ${Sr}_{n + 1} {Ir}_{n} O_{3 n + 1}$ $(n = 1, 2)$ iridates probed by x-ray Raman spectroscopy
journal, August 2014

Interference of second harmonics due to electric and magnetic dipoles in antiferromagnetic ${Cr}_{2} O_{3}$
journal, October 1998

Optical dichroism: E1–M1 integral relations
journal, February 2006

Orbital-dependent polaron formation in the relativistic Mott insulator ${Sr}_{2} {IrO}_{4}$
journal, July 2014

Resonant x-ray diffraction: multipole interpretation
journal, March 2012

Resonant x-ray scattering as a probe of toroidal moments in centrosymmetric systems
journal, October 2004

Anisotropic magnetization-induced second harmonic generation in Fe/Au superlattices
journal, October 2001

Non-Fermi-liquid states and pairing instability of a general model of copper oxide metals
journal, June 1997

Second-harmonic generation as a tool for studying electronic and magnetic structures of crystals: review
journal, January 2005

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

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

Femtosecond switching of magnetism via strongly correlated spin–charge quantum excitations
journal, April 2013

Symmetry considerations for detection of time-reversal breaking phases in cuprates by x-ray diffraction and absorption
journal, April 2003

Robustness of Basal-Plane Antiferromagnetic Order and the $J_{eff} = 1 / 2$ State in Single-Layer Iridate Spin-Orbit Mott Insulators
journal, March 2013

Giant magnetoelectric effect in the $J_{eff} = \frac{1}{2}$ Mott insulator ${Sr}_{2} {IrO}_{4}$
journal, October 2009

Dilute magnetism and spin-orbital percolation effects in ${Sr}_{2}$ ${Ir}_{1 - x}$ ${Rh}_{x}$ $O_{4}$
journal, February 2014

Locking of iridium magnetic moments to the correlated rotation of oxygen octahedra in Sr ₂ IrO ₄ revealed by x-ray resonant scattering
journal, September 2013

Electronic structures of layered perovskite ${Sr}_{2} M O_{4}$ ( $M = Ru$ , Rh, and Ir)
journal, September 2006

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

Interplay of many-body and single-particle interactions in iridates and rhodates
journal, January 2014

X-Ray Magnetochiral Dichroism: A New Spectroscopic Probe of Parity Nonconserving Magnetic Solids
journal, May 2002

Observation of a $d$-wave gap in electron-doped Sr$_2$IrO$_4$
text, January 2015

Disentangling multipole resonances through a full x-ray polarization analysis
text, January 2006

Direct experimental observation of the molecular J eff = 3/2 ground state in the lacunar spinel GaTa4Se8
journal, October 2017

Sr ₅ Os ₃ O ₁₃ : a mixed valence osmium( v , vi ) layered perovskite variant exhibiting temperature dependent charge distribution
journal, January 2018

Magnetic hexadecapole order and magnetopiezoelectric metal state in ${Ba}_{1 - x} K_{x} {Mn}_{2} {As}_{2}$
journal, August 2017