Influence of electron doping on the ground state of (Sr1-xLax)2IrO4

Chen, Xiang; Hogan, Tom; Walkup, D.; Zhou, Wenwen; Pokharel, M.; Yao, Mengliang; Tian, Wei; Ward, Thomas Zac; Zhao, Y.; Parshall, Dr. D.; Opeil, C.; Lynn, J. W.; Madhavan, Vidya; Wilson, Stephen

doi:10.1103/PhysRevB.92.075125

Title: Influence of electron doping on the ground state of (Sr_1-xLa_x)₂IrO₄

Abstract

The evolution of the electronic properties of electron-doped (Sr_1-xLa_x)₂IrO₄ is experimentally explored as the doping limit of La is approached. As electrons are introduced, the electronic ground state transitions from a spin-orbit Mott phase into an electronically phase separated state, where long-range magnetic order vanishes beyond x = 0:02 and charge transport remains percolative up to the limit of La substitution (x =0:06). In particular, the electronic ground state remains inhomogeneous even beyond the collapse of the parent state's long-range antiferromagnetic order, while persistent short-range magnetism survives up to the highest La-substitution levels. Furthermore, as electrons are doped into Sr₂IrO₄, we observe the appearance of a low temperature magnetic glass-like state intermediate to the complete suppression of antiferromagnetic order. Universalities and di erences in the electron-doped phase diagrams of single layer and bilayer Ruddlesden-Popper strontium iridates are discussed.

Authors:

Chen, Xiang ^[1]; Hogan, Tom ^[1]; Walkup, D. ^[2]; Zhou, Wenwen ^[2]; Pokharel, M. ^[2]; Yao, Mengliang ^[2]; Tian, Wei ^[3]; Ward, Thomas Zac ^[3]; Zhao, Y. ^[4]; Parshall, Dr. D. ^[5]; Opeil, C. ^[2]; Lynn, J. W. ^[6]; Madhavan, Vidya ^[7]; Wilson, Stephen ^[1]

Univ. of California, Santa Barbara, CA (United States)
Boston College, Chestnut Hill, MA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Univ. of Illinois, Urbana-Champaign, IL (United States)

Publication Date:: Mon Aug 17 00:00:00 EDT 2015

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1286907

Alternate Identifier(s):: OSTI ID: 1211566

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review. B, Condensed Matter and Materials Physics

Additional Journal Information:: Journal Volume: 92; Journal Issue: 7; Journal ID: ISSN 1098-0121

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Chen, Xiang, Hogan, Tom, Walkup, D., Zhou, Wenwen, Pokharel, M., Yao, Mengliang, Tian, Wei, Ward, Thomas Zac, Zhao, Y., Parshall, Dr. D., Opeil, C., Lynn, J. W., Madhavan, Vidya, and Wilson, Stephen. Influence of electron doping on the ground state of (Sr1-xLax)2IrO4.  United States: N. p., 2015. 
Web.  doi:10.1103/PhysRevB.92.075125.

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                    Chen, Xiang, Hogan, Tom, Walkup, D., Zhou, Wenwen, Pokharel, M., Yao, Mengliang, Tian, Wei, Ward, Thomas Zac, Zhao, Y., Parshall, Dr. D., Opeil, C., Lynn, J. W., Madhavan, Vidya, & Wilson, Stephen. Influence of electron doping on the ground state of (Sr1-xLax)2IrO4.  United States.  https://doi.org/10.1103/PhysRevB.92.075125

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                    Chen, Xiang, Hogan, Tom, Walkup, D., Zhou, Wenwen, Pokharel, M., Yao, Mengliang, Tian, Wei, Ward, Thomas Zac, Zhao, Y., Parshall, Dr. D., Opeil, C., Lynn, J. W., Madhavan, Vidya, and Wilson, Stephen. Mon .  
"Influence of electron doping on the ground state of (Sr1-xLax)2IrO4".  United States.  https://doi.org/10.1103/PhysRevB.92.075125.  https://www.osti.gov/servlets/purl/1286907.

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@article{osti_1286907,

  title        = {Influence of electron doping on the ground state of (Sr1-xLax)2IrO4},

  author       = {Chen, Xiang and Hogan, Tom and Walkup, D. and Zhou, Wenwen and Pokharel, M. and Yao, Mengliang and Tian, Wei and Ward, Thomas Zac and Zhao, Y. and Parshall, Dr. D. and Opeil, C. and Lynn, J. W. and Madhavan, Vidya and Wilson, Stephen},

  abstractNote = {The evolution of the electronic properties of electron-doped (Sr1-xLax)2IrO4 is experimentally explored as the doping limit of La is approached. As electrons are introduced, the electronic ground state transitions from a spin-orbit Mott phase into an electronically phase separated state, where long-range magnetic order vanishes beyond x = 0:02 and charge transport remains percolative up to the limit of La substitution (x =0:06). In particular, the electronic ground state remains inhomogeneous even beyond the collapse of the parent state's long-range antiferromagnetic order, while persistent short-range magnetism survives up to the highest La-substitution levels. Furthermore, as electrons are doped into Sr2IrO4, we observe the appearance of a low temperature magnetic glass-like state intermediate to the complete suppression of antiferromagnetic order. Universalities and di erences in the electron-doped phase diagrams of single layer and bilayer Ruddlesden-Popper strontium iridates are discussed.},

  doi          = {10.1103/PhysRevB.92.075125},

  journal      = {Physical Review. B, Condensed Matter and Materials Physics},

  number       = 7,

  volume       = 92,

  place        = {United States},

  year         = {Mon Aug 17 00:00:00 EDT 2015},

  month        = {Mon Aug 17 00:00:00 EDT 2015}

}

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Sr₂IrO₄ is a spin-orbit coupled insulator with an antiferromagnetic (AFM) transition at TN=240 K. We report results of a comprehensive study of single-crystal Sr₂Ir_1-xTb_xO₄ (0 x 0.03). This study found that mere 3% (x=0.03) tetravalent Tb⁴⁺(4f⁷) substituting for Ir⁴⁺ (rather than Sr²⁺) completely suppresses the long-range AFM transition but stabilizes the insulating state, leading to a phase diagram featuring a decoupling of magnetic interactions and charge gap. The insulating state at x=0.03 is characterized by an unusually large specific heat at low temperatures and an incommensurate magnetic state having a magnetic peak at (0.95, 0, 0) in the neutron diffraction.more »« less
Cited by 40
https://doi.org/10.1103/PhysRevB.92.214411

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Structural and magnetic properties of the single-layer manganese oxide La{sub 1-x}Sr{sub 1+x}MnO{sub 4}

Journal Article Larochelle, S ; Vajk, O P ; Mehta, A ; ... - Physical Review. B, Condensed Matter and Materials Physics

Using x-ray and neutron scattering, we have studied the structural and magnetic properties of the single-layer manganite La{sub 1-x}Sr{sub 1+x}MnO{sub 4}(0{<=}x<0.7). Single crystals were grown by the floating-zone method at 18 La/Sr concentrations. The low-temperature phase diagram can be understood by considering the strong coupling of the magnetic and orbital degrees of freedom, and it can be divided into three distinct regions: low (x<0.12), intermediate (0.12{<=}x<0.45), and high (x{>=}0.45) doping. LaSrMnO{sub 4}(x=0) is an antiferromagnetic Mott insulator, and its spin-wave spectrum is well described by linear spin-wave theory for the spin-2 square-lattice Heisenberg Hamiltonian with Ising anisotropy. Upon doping, asmore »« less
https://doi.org/10.1103/PhysRevB.71.024435

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Title: Influence of electron doping on the ground state of (Sr1-xLax)2IrO4

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Citation Formats

Transverse magnetoresistance in AgMn in the spin glass regime journal, January 1979

Imaging the evolution of metallic states in a correlated iridate journal, May 2013

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

Double-Focusing Thermal Triple-Axis Spectrometer at the NCNR journal, January 2012

Anomalous behavior of the magnetoresistance of NiMn alloys in the spin‐glass and ferromagnetic states journal, March 1984

Conduction in non-crystalline systems IX. the minimum metallic conductivity journal, October 1972

Effects of doping on the lattice parameter of SrTiO 3 journal, June 2012

Atomically resolved spectroscopic study of Sr2IrO4: Experiment and theory journal, October 2013

Anomalous magnetoresistance in AuFe spin glass journal, March 1979

Coulomb gap and low temperature conductivity of disordered systems journal, February 1975

Transport and thermal properties of weakly ferromagnetic Sr 2 IrO 4 journal, August 2006

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

Carrier localization and electronic phase separation in a doped spin-orbit-driven Mott phase in Sr3(Ir1–xRux)2O7 journal, February 2014

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

Dimensionality-Controlled Insulator-Metal Transition and Correlated Metallic State in 5 d Transition Metal Oxides Sr n + 1 Ir n O 3 n + 1 ( n = 1 , 2, and ∞ ) journal, November 2008

Twisted Hubbard Model for Sr 2 IrO 4 : Magnetism and Possible High Temperature Superconductivity journal, March 2011

Monte Carlo Study of an Unconventional Superconducting Phase in Iridium Oxide J eff = 1 / 2 Mott Insulators Induced by Carrier Doping journal, January 2013

Instantaneous spin correlations in La 2 CuO 4 journal, June 1999

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

Local density of states study of a spin-orbit-coupling induced Mott insulator Sr 2 Ir O 4 journal, July 2014

Tunneling into the Mott insulator Sr 2 IrO 4 journal, February 2014

Weak ferromagnetism, metal-to-nonmetal transition, and negative differential resistivity in single-crystal Sr 2 IrO 4 journal, May 1998

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

Theoretical study of insulating mechanism in multiorbital Hubbard models with a large spin-orbit coupling: Slater versus Mott scenario in Sr 2 IrO 4 journal, April 2014

Ab initio Studies on the Interplay between Spin-Orbit Interaction and Coulomb Correlation in Sr 2 IrO 4 and Ba 2 IrO 4 journal, February 2012

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

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

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

Anisotropic exchange interactions of spin-orbit-integrated states in Sr 2 IrO 4 journal, August 2009

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

Lattice-driven magnetoresistivity and metal-insulator transition in single-layered iridates journal, September 2011

Spin ordering and electronic texture in the bilayer iridate Sr 3 Ir 2 O 7 journal, September 2012

Anomalous magnetic and transport behavior in the magnetic insulator Sr 3 Ir 2 O 7 journal, December 2002

Evidence for ordered magnetic moments at oxygen sites in antiferromagnetic Sr 2 IrO 4 and Sr 3 Ir 2 O 7 journal, April 2015

Electron-doped Sr 2 IrO 4 − δ ( 0 ≤ δ ≤ 0.04 ) : Evolution of a disordered J eff = 1 2 Mott insulator into an exotic metallic state journal, September 2010

First-Order Melting of a Weak Spin-Orbit Mott Insulator into a Correlated Metal journal, June 2015

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

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

Intergranular Giant Magnetoresistance in a Spontaneously Phase Separated Perovskite Oxide journal, January 2005

Hopping Conductivity in Granular Metals journal, July 1973

Spin glasses: Experimental facts, theoretical concepts, and open questions journal, October 1986

Spin glasses: Some recent experiments journal, December 1986

Scaling Theory of Localization: Absence of Quantum Diffusion in Two Dimensions journal, March 1979

Electronic properties of two-dimensional systems journal, April 1982

Mobility of the Doped Holes and the Antiferromagnetic Correlations in Underdoped High- T c Cuprates journal, June 2001

Magnetic, transport, and optical properties of monolayer copper oxides journal, July 1998

Gate-defined Josephson junctions in magic-angle twisted bilayer graphene journal, May 2021

Atomically resolved spectroscopic study of Sr2IrO4: Experiment and theory text, January 2013

Mobility of the Doped Holes and the Antiferromagnetic Correlations in Underdoped High-Tc Cuprates text, January 2001

Spin ordering and electronic texture in the bilayer iridate Sr$_3$Ir$_2$O$_7$ text, January 2012

Monte Carlo study of an unconventional superconducting phase in Ir-oxide J_{eff}=1/2 Mott insulators induced by carrier doping text, January 2012

Instantaneous Spin Correlations in La2CuO4 text, January 1999

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

Unidirectional spin density wave state in metallic (Sr1−xLax)2IrO4 journal, January 2018

The challenge of spin–orbit-tuned ground states in iridates: a key issues review journal, February 2018

Correlation transports at p- / n- types in electron metastable perovskite family of rare-earth nickelates journal, February 2020

Quasistatic antiferromagnetism in the quantum wells of SmTiO3/SrTiO3 heterostructures journal, February 2018

Two dimensional electron gas in the $\delta$ -doped iridates with strong spin–orbit coupling: La$_\delta$ Sr 2 IrO 4 journal, July 2019

Atomic-scale fragmentation and collapse of antiferromagnetic order in a doped Mott insulator journal, October 2019

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

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

Synthesis and physical properties of the new iridium oxyfluoride S r 2 Ir ( O , F ) 6 − δ using a topochemical reaction method journal, January 2020

Structure, magnetism, and transport properties for Ca doping in Sr 2 IrO 4 journal, May 2017

Decoupling of magnetism and electric transport in single-crystal (Sr1-xAx)2IrO4 (A = Ca or Ba) text, January 2017

Stability of the Antiferromagnetic State in the Electron Doped Iridates text, January 2018

Atomic-scale fragmentation and collapse of antiferromagnetic order in a doped Mott insulator text, January 2019

The Jeff=1/2 antiferromagnet Sr2IrO4: A golden avenue toward new physics and functions text, January 2021

Title: Influence of electron doping on the ground state of (Sr_1-xLa_x)₂IrO₄

Transverse magnetoresistance in AgMn in the spin glass regime
journal, January 1979

Imaging the evolution of metallic states in a correlated iridate
journal, May 2013

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

Double-Focusing Thermal Triple-Axis Spectrometer at the NCNR
journal, January 2012

Anomalous behavior of the magnetoresistance of NiMn alloys in the spin‐glass and ferromagnetic states
journal, March 1984

Conduction in non-crystalline systems IX. the minimum metallic conductivity
journal, October 1972

Effects of doping on the lattice parameter of SrTiO ₃
journal, June 2012

Atomically resolved spectroscopic study of Sr2IrO4: Experiment and theory
journal, October 2013

Anomalous magnetoresistance in AuFe spin glass
journal, March 1979

Coulomb gap and low temperature conductivity of disordered systems
journal, February 1975

Transport and thermal properties of weakly ferromagnetic Sr ₂ IrO ₄
journal, August 2006

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

Carrier localization and electronic phase separation in a doped spin-orbit-driven Mott phase in Sr3(Ir1–xRux)2O7
journal, February 2014

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

Dimensionality-Controlled Insulator-Metal Transition and Correlated Metallic State in $5 d$ Transition Metal Oxides ${Sr}_{n + 1} {Ir}_{n} O_{3 n + 1}$ ( $n = 1$ , 2, and $\infty$ )
journal, November 2008

Twisted Hubbard Model for ${Sr}_{2} {IrO}_{4}$ : Magnetism and Possible High Temperature Superconductivity
journal, March 2011

Monte Carlo Study of an Unconventional Superconducting Phase in Iridium Oxide $J_{eff} = 1 / 2$ Mott Insulators Induced by Carrier Doping
journal, January 2013

Instantaneous spin correlations in ${La}_{2} {CuO}_{4}$
journal, June 1999

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

Local density of states study of a spin-orbit-coupling induced Mott insulator ${Sr}_{2} Ir O_{4}$
journal, July 2014

Tunneling into the Mott insulator ${Sr}_{2}$ ${IrO}_{4}$
journal, February 2014

Weak ferromagnetism, metal-to-nonmetal transition, and negative differential resistivity in single-crystal ${Sr}_{2} {IrO}_{4}$
journal, May 1998

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

Theoretical study of insulating mechanism in multiorbital Hubbard models with a large spin-orbit coupling: Slater versus Mott scenario in ${Sr}_{2}$ ${IrO}_{4}$
journal, April 2014

Ab initio Studies on the Interplay between Spin-Orbit Interaction and Coulomb Correlation in ${Sr}_{2} {IrO}_{4}$ and ${Ba}_{2} {IrO}_{4}$
journal, February 2012

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

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

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

Anisotropic exchange interactions of spin-orbit-integrated states in ${Sr}_{2} {IrO}_{4}$
journal, August 2009

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

Lattice-driven magnetoresistivity and metal-insulator transition in single-layered iridates
journal, September 2011

Spin ordering and electronic texture in the bilayer iridate Sr $_{3}$ Ir $_{2}$ O $_{7}$
journal, September 2012

Anomalous magnetic and transport behavior in the magnetic insulator ${Sr}_{3} {Ir}_{2} O_{7}$
journal, December 2002

Evidence for ordered magnetic moments at oxygen sites in antiferromagnetic ${Sr}_{2} {IrO}_{4}$ and ${Sr}_{3} {Ir}_{2} O_{7}$
journal, April 2015

Electron-doped ${Sr}_{2} {IrO}_{4 - δ}$ $(0 \leq δ \leq 0.04)$ : Evolution of a disordered $J_{eff} = \frac{1}{2}$ Mott insulator into an exotic metallic state
journal, September 2010

First-Order Melting of a Weak Spin-Orbit Mott Insulator into a Correlated Metal
journal, June 2015

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

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

Intergranular Giant Magnetoresistance in a Spontaneously Phase Separated Perovskite Oxide
journal, January 2005

Hopping Conductivity in Granular Metals
journal, July 1973

Spin glasses: Experimental facts, theoretical concepts, and open questions
journal, October 1986

Spin glasses: Some recent experiments
journal, December 1986

Scaling Theory of Localization: Absence of Quantum Diffusion in Two Dimensions
journal, March 1979

Electronic properties of two-dimensional systems
journal, April 1982

Mobility of the Doped Holes and the Antiferromagnetic Correlations in Underdoped High- $T_{c}$ Cuprates
journal, June 2001

Magnetic, transport, and optical properties of monolayer copper oxides
journal, July 1998

Gate-defined Josephson junctions in magic-angle twisted bilayer graphene
journal, May 2021

Atomically resolved spectroscopic study of Sr2IrO4: Experiment and theory
text, January 2013

Mobility of the Doped Holes and the Antiferromagnetic Correlations in Underdoped High-Tc Cuprates
text, January 2001

Spin ordering and electronic texture in the bilayer iridate Sr$_3$Ir$_2$O$_7$
text, January 2012

Monte Carlo study of an unconventional superconducting phase in Ir-oxide J_{eff}=1/2 Mott insulators induced by carrier doping
text, January 2012

Instantaneous Spin Correlations in La2CuO4
text, January 1999

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

Unidirectional spin density wave state in metallic (Sr1−xLax)2IrO4
journal, January 2018

The challenge of spin–orbit-tuned ground states in iridates: a key issues review
journal, February 2018

Correlation transports at p- / n- types in electron metastable perovskite family of rare-earth nickelates
journal, February 2020

Quasistatic antiferromagnetism in the quantum wells of SmTiO3/SrTiO3 heterostructures
journal, February 2018

Two dimensional electron gas in the $\delta$ -doped iridates with strong spin–orbit coupling: La$_\delta$ Sr ₂ IrO ₄
journal, July 2019

Atomic-scale fragmentation and collapse of antiferromagnetic order in a doped Mott insulator
journal, October 2019

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

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

Synthesis and physical properties of the new iridium oxyfluoride $S r_{2} Ir {(O, F)}_{6 - δ}$ using a topochemical reaction method
journal, January 2020

Structure, magnetism, and transport properties for Ca doping in Sr ₂ IrO ₄
journal, May 2017

Decoupling of magnetism and electric transport in single-crystal (Sr1-xAx)2IrO4 (A = Ca or Ba)
text, January 2017

Stability of the Antiferromagnetic State in the Electron Doped Iridates
text, January 2018

Atomic-scale fragmentation and collapse of antiferromagnetic order in a doped Mott insulator
text, January 2019

The Jeff=1/2 antiferromagnet Sr2IrO4: A golden avenue toward new physics and functions
text, January 2021