Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr2IrO4: A study of Sr2Ir1–xMxO4 (M=Fe or Co)

Hu, Bing; Zhao, Hengdi; Zhang, Yu; Schlottmann, Pedro; Ye, Feng; Cao, Gang

doi:10.1103/physrevb.103.115122

Title: Correlation between antiferromagnetic and Mott states in spin orbit coupled ${Sr}_{2} Ir O_{4}$ : A study of ${Sr}_{2} {Ir}_{1 - x} M_{x} O_{4}$ ( $M = Fe$ or Co)

Abstract

Sr₂IrO₄ is an archetypal spin-orbit-coupled Mott insulator with an antiferromagnetic state below 240 K. Here we report results of our study on single crystals of Sr₂Ir_1–xFe_xO₄ (0 ≤ x < 0.32) and Sr₂Ir_1–xCo_xO₄ (0 ≤ x < 0.22). Fe doping retains the antiferromagnetic state but simultaneously precipitates an emergent metallic state whereas Co doping causes a rapid collapse of both the antiferromagnetic and Mott states, giving rise to a confined metallic state featuring a pronounced linearity of the basal-plane resistivity up to 700 K. The results indicate tetravalent Fe⁴⁺ (3d⁴) ions in the intermediate spin state with S = 1 and Co⁴⁺ (3d⁵) ions in the high spin state with S = 5/2 substituting for Ir⁴⁺ (5d⁵) ions in Sr₂IrO₄, respectively. The effective magnetic moment closely tracks the Néel temperature as doping increases, suggesting that the spin state of the dopant predominately determines the magnetic properties in doped Sr₂IrO₄. Furthermore, all relevant properties including charge-carrier density (e.g., 10²⁸/m³), Sommerfeld coefficient (e.g., 19 mJ / mole K²), and Wilson ratio (e.g., 2.6) consistently demonstrate an emergent metallic state that is both robust and highly correlated in the two systems, arising from the percolation of bound states and the weakening of structuralmore »« less

Authors:

^[1]; Zhao, Hengdi ^[2]; Zhang, Yu ^[2];

^[3];

^[4];

^[2]

Univ. of Colorado, Boulder, CO (United States); North China Electric Power University, Beijing (China)
Univ. of Colorado, Boulder, CO (United States)
Florida State Univ., Tallahassee, FL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Mon Mar 15 00:00:00 EDT 2021

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE; National Science Foundation (NSF)

OSTI Identifier:: 1819586

Grant/Contract Number:: AC05-00OR22725; DMR-1903888

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 103; Journal Issue: 11; 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; Antiferromagnetism; Magnetic anisotropy; Metal-insulator transition; Spin-orbit coupling; Mott insulators

Citation Formats


                    Hu, Bing, Zhao, Hengdi, Zhang, Yu, Schlottmann, Pedro, Ye, Feng, and Cao, Gang. Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr2IrO4: A study of Sr2Ir1–xMxO4 (M=Fe or Co).  United States: N. p., 2021. 
Web.  doi:10.1103/physrevb.103.115122.

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                    Hu, Bing, Zhao, Hengdi, Zhang, Yu, Schlottmann, Pedro, Ye, Feng, & Cao, Gang. Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr2IrO4: A study of Sr2Ir1–xMxO4 (M=Fe or Co).  United States.  https://doi.org/10.1103/physrevb.103.115122

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                    Hu, Bing, Zhao, Hengdi, Zhang, Yu, Schlottmann, Pedro, Ye, Feng, and Cao, Gang. Mon .  
"Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr2IrO4: A study of Sr2Ir1–xMxO4 (M=Fe or Co)".  United States.  https://doi.org/10.1103/physrevb.103.115122.  https://www.osti.gov/servlets/purl/1819586.

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@article{osti_1819586,

  title        = {Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr2IrO4: A study of Sr2Ir1–xMxO4 (M=Fe or Co)},

  author       = {Hu, Bing and Zhao, Hengdi and Zhang, Yu and Schlottmann, Pedro and Ye, Feng and Cao, Gang},

  abstractNote = {Sr2IrO4 is an archetypal spin-orbit-coupled Mott insulator with an antiferromagnetic state below 240 K. Here we report results of our study on single crystals of Sr2Ir1–xFexO4 (0 ≤ x < 0.32) and Sr2Ir1–xCoxO4 (0 ≤ x < 0.22). Fe doping retains the antiferromagnetic state but simultaneously precipitates an emergent metallic state whereas Co doping causes a rapid collapse of both the antiferromagnetic and Mott states, giving rise to a confined metallic state featuring a pronounced linearity of the basal-plane resistivity up to 700 K. The results indicate tetravalent Fe4+ (3d4) ions in the intermediate spin state with S = 1 and Co4+ (3d5) ions in the high spin state with S = 5/2 substituting for Ir4+ (5d5) ions in Sr2IrO4, respectively. The effective magnetic moment closely tracks the Néel temperature as doping increases, suggesting that the spin state of the dopant predominately determines the magnetic properties in doped Sr2IrO4. Furthermore, all relevant properties including charge-carrier density (e.g., 1028/m3), Sommerfeld coefficient (e.g., 19 mJ / mole K2), and Wilson ratio (e.g., 2.6) consistently demonstrate an emergent metallic state that is both robust and highly correlated in the two systems, arising from the percolation of bound states and the weakening of structural distortions. Furthermore, this study strongly indicates that the antiferromagnetic and Mott states are correlated in an unconventional manner in Sr2IrO4.},

  doi          = {10.1103/physrevb.103.115122},

  journal      = {Physical Review B},

  number       = 11,

  volume       = 103,

  place        = {United States},

  year         = {Mon Mar 15 00:00:00 EDT 2021},

  month        = {Mon Mar 15 00:00:00 EDT 2021}

}

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Title: Correlation between antiferromagnetic and Mott states in spin orbit coupled Sr 2 Ir O 4 : A study of Sr 2 Ir 1 – x M x O 4 ( M = Fe or Co)

Abstract

Citation Formats

X-ray Absorption Spectroscopy Study of the Effect of Rh doping in Sr2IrO4 journal, March 2016

Spin-orbit tuned metal-insulator transitions in single-crystal Sr 2 Ir 1 − x Rh x O 4 ( 0 ≤ x ≤ 1 ) journal, September 2012

Novel metallic ferromagnet Sr2CoO4 journal, August 2005

Superconductivity in doped Sr 2 IrO 4 : A functional renormalization group study journal, March 2014

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

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

Correlated Quantum Phenomena in the Strong Spin-Orbit Regime journal, March 2014

Pseudospin-lattice coupling and electric control of the square-lattice iridate Sr 2 Ir O 4 journal, September 2020

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

Interlayer pair hopping: Superconductivity from the resonating-valence-bond state journal, April 1988

Coulomb correlations in 4d and 5d oxides from first principles—or how spin–orbit materials choose their effective orbital degeneracies journal, May 2017

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

Large linear-in-temperature resistivity in twisted bilayer graphene journal, August 2019

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

Possible Quantum Paramagnetism in Compressed Sr 2 IrO 4 journal, February 2020

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

Dimensionality-controlled Mott transition and correlation effects in single-layer and bilayer perovskite iridates journal, June 2013

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

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

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

Neutron Powder Diffraction Study of the Crystal Structures of Sr2RuO4 and Sr2IrO4 at Room Temperature and at 10 K journal, October 1994

From J eff = 1 / 2 insulator to p -wave superconductor in single-crystal S r 2 I r 1 − x R u x O 4 ( 0 ≤ x ≤ 1 ) journal, December 2015

Odd-parity superconductivity driven by octahedra rotations in iridium oxides journal, August 2019

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

Odd-Parity Triplet Superconducting Phase in Multiorbital Materials with a Strong Spin-Orbit Coupling: Application to Doped Sr 2 IrO 4 journal, October 2014

Decoupling of the antiferromagnetic and insulating states in Tb-doped S r 2 Ir O 4 journal, December 2015

Why the temperature is high journal, July 2004

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

Metal-insulator transition in dirty Kondo insulators journal, January 1996

Hallmarks of the Mott-metal crossover in the hole-doped pseudospin-1/2 Mott insulator Sr2IrO4 journal, April 2016

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

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

Persistent insulating state at megabar pressures in strongly spin-orbit coupled S r 2 Ir O 4 journal, April 2020

Recent progress on correlated electron systems with strong spin–orbit coupling journal, August 2016

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

Superconductivity in Bad Metals journal, April 1995

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

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

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

Pressure-Induced Confined Metal from the Mott Insulator Sr 3 Ir 2 O 7 journal, May 2016

‘Confined coherence’ in strongly correlated anisotropic metals journal, December 1997

Localized-to-itinerant electron transition in Sr 2 Ir 1 − x Ru x O 4 journal, May 1994

Influence of electron doping on the ground state of ( Sr 1 − x La x ) 2 IrO 4 journal, August 2015

Sr 2 Ir 1 − x Rh x O 4 ( x < 0.5 ) : An inhomogeneous j eff = 1 2 Hubbard system journal, August 2015

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

Synthesis and characterization of Sr2Ir1−xMxO4 (M=Ti, Fe, Co) solid solutions journal, June 2012

Title: Correlation between antiferromagnetic and Mott states in spin orbit coupled ${Sr}_{2} Ir O_{4}$ : A study of ${Sr}_{2} {Ir}_{1 - x} M_{x} O_{4}$ ( $M = Fe$ or Co)

X-ray Absorption Spectroscopy Study of the Effect of Rh doping in Sr2IrO4
journal, March 2016

Spin-orbit tuned metal-insulator transitions in single-crystal Sr $_{2}$ Ir $_{1 - x}$ Rh $_{x}$ O $_{4}$ ( $0 \leq x \leq 1$ )
journal, September 2012

Novel metallic ferromagnet Sr2CoO4
journal, August 2005

Superconductivity in doped ${Sr}_{2} {IrO}_{4}$ : A functional renormalization group study
journal, March 2014

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

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

Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014

Pseudospin-lattice coupling and electric control of the square-lattice iridate ${Sr}_{2} Ir O_{4}$
journal, September 2020

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

Interlayer pair hopping: Superconductivity from the resonating-valence-bond state
journal, April 1988

Coulomb correlations in 4d and 5d oxides from first principles—or how spin–orbit materials choose their effective orbital degeneracies
journal, May 2017

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

Large linear-in-temperature resistivity in twisted bilayer graphene
journal, August 2019

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

Possible Quantum Paramagnetism in Compressed ${Sr}_{2} {IrO}_{4}$
journal, February 2020

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

Dimensionality-controlled Mott transition and correlation effects in single-layer and bilayer perovskite iridates
journal, June 2013

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

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

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

Neutron Powder Diffraction Study of the Crystal Structures of Sr2RuO4 and Sr2IrO4 at Room Temperature and at 10 K
journal, October 1994

From $J_{eff} = 1 / 2$ insulator to $p$ -wave superconductor in single-crystal $S r_{2} I r_{1 - x} R u_{x} O_{4} (0 \leq x \leq 1)$
journal, December 2015

Odd-parity superconductivity driven by octahedra rotations in iridium oxides
journal, August 2019

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

Odd-Parity Triplet Superconducting Phase in Multiorbital Materials with a Strong Spin-Orbit Coupling: Application to Doped ${Sr}_{2} {IrO}_{4}$
journal, October 2014

Decoupling of the antiferromagnetic and insulating states in Tb-doped $S r_{2} Ir O_{4}$
journal, December 2015

Why the temperature is high
journal, July 2004

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

Metal-insulator transition in dirty Kondo insulators
journal, January 1996

Hallmarks of the Mott-metal crossover in the hole-doped pseudospin-1/2 Mott insulator Sr2IrO4
journal, April 2016

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

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

Persistent insulating state at megabar pressures in strongly spin-orbit coupled $S r_{2} Ir O_{4}$
journal, April 2020

Recent progress on correlated electron systems with strong spin–orbit coupling
journal, August 2016

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

Superconductivity in Bad Metals
journal, April 1995

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

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

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

Pressure-Induced Confined Metal from the Mott Insulator ${Sr}_{3} {Ir}_{2} O_{7}$
journal, May 2016

‘Confined coherence’ in strongly correlated anisotropic metals
journal, December 1997

Localized-to-itinerant electron transition in ${Sr}_{2}$ ${Ir}_{1 - x}$ ${Ru}_{x}$ $O_{4}$
journal, May 1994

Influence of electron doping on the ground state of $({Sr}_{1 - x} {La}_{x})_{2} {IrO}_{4}$
journal, August 2015

${Sr}_{2} {Ir}_{1 - x} {Rh}_{x} O_{4} (x < 0.5)$ : An inhomogeneous $j_{eff} = \frac{1}{2}$ Hubbard system
journal, August 2015

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

Synthesis and characterization of Sr2Ir1−xMxO4 (M=Ti, Fe, Co) solid solutions
journal, June 2012