Strain-induced high-temperature perovskite ferromagnetic insulator

doi:10.1073/pnas.1707817115

Title: Strain-induced high-temperature perovskite ferromagnetic insulator

Abstract

Ferromagnetic insulators are required for many new magnetic devices, such as dissipationless quantum-spintronic devices, magnetic tunneling junctions, etc. Ferromagnetic insulators with a high Curie temperature and a high-symmetry structure are critical integration with common single-crystalline oxide films or substrates. So far, the commonly used ferromagnetic insulators mostly possess low-symmetry structures associated with a poor growth quality and widespread properties. The few known high-symmetry materials either have extremely low Curie temperatures (≤16 K), or require chemical doping of an otherwise antiferromagnetic matrix. Here we present compelling evidence that the LaCoO₃ single-crystalline thin film under tensile strain is a rare undoped perovskite ferromagnetic insulator with a remarkably high T_C of up to 90 K. Both experiments and first-principles calculations demonstrate tensile-strain-induced ferromagnetism which does not exist in bulk LaCoO₃. The ferromagnetism is strongest within a nearly stoichiometric structure, disappearing when the Co²⁺ defect concentration reaches about 10%. Furthermore, significant impact of the research includes demonstration of a strain-induced high-temperature ferromagnetic insulator, successful elevation of the transition over the liquid-nitrogen temperature, and high potential for integration into large-area device fabrication processes.

Authors:

Meng, Dechao ^[1]; Guo, Hongli ^[2]; Cui, Zhangzhang ^[3]; Ma, Chao ^[1]; Zhao, Jin ^[1]; Lu, Jiangbo ^[4]; Xu, Hui ^[1]; Wang, Zhicheng ^[1]; Hu, Xiang ^[1]; Fu, Zhengping ^[1]; Peng, Ranran ^[1]; Guo, Jinghua ^[5]; Zhai, Xiaofang ^[1]; Brown, Gail J. ^[6]; Knize, Randy ^[7]; Lu, Yalin ^[8]

Univ. of Science and Technology of China, Anhui (People's Republic of China)
Univ. of Science and Technology of China, Anhui (People's Republic of China); Chinese Academy of Sciences, Anhui (People's Republic of China)
Univ. of Science and Technology of China, Anhui (People's Republic of China); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Shaanxi Normal Univ., Shaanxi (People's Republic of China)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)
Wright-Patterson Air Force Base (AFB), Wright-Patterson AFB, OH (United States)
US Air Force Academy, CO (United States)
Univ. of Science and Technology of China, Anhui (People's Republic of China); Wright-Patterson Air Force Base (AFB), Wright-Patterson AFB, OH (United States); US Air Force Academy, CO (United States)

Publication Date:: 2018-03-05

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1465448

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:: Journal Volume: 115; Journal Issue: 12; Related Information: © 2018 National Academy of Sciences. All rights reserved.; Journal ID: ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; ferromagnetic insulator; strain; defect; pulsed-laser deposition; X-ray absorption

Citation Formats


                    Meng, Dechao, Guo, Hongli, Cui, Zhangzhang, Ma, Chao, Zhao, Jin, Lu, Jiangbo, Xu, Hui, Wang, Zhicheng, Hu, Xiang, Fu, Zhengping, Peng, Ranran, Guo, Jinghua, Zhai, Xiaofang, Brown, Gail J., Knize, Randy, and Lu, Yalin. Strain-induced high-temperature perovskite ferromagnetic insulator.  United States: N. p., 2018. 
        Web.  doi:10.1073/pnas.1707817115.

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                    Meng, Dechao, Guo, Hongli, Cui, Zhangzhang, Ma, Chao, Zhao, Jin, Lu, Jiangbo, Xu, Hui, Wang, Zhicheng, Hu, Xiang, Fu, Zhengping, Peng, Ranran, Guo, Jinghua, Zhai, Xiaofang, Brown, Gail J., Knize, Randy, & Lu, Yalin. Strain-induced high-temperature perovskite ferromagnetic insulator.  United States.  doi:10.1073/pnas.1707817115.

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                    Meng, Dechao, Guo, Hongli, Cui, Zhangzhang, Ma, Chao, Zhao, Jin, Lu, Jiangbo, Xu, Hui, Wang, Zhicheng, Hu, Xiang, Fu, Zhengping, Peng, Ranran, Guo, Jinghua, Zhai, Xiaofang, Brown, Gail J., Knize, Randy, and Lu, Yalin. Mon .  
        "Strain-induced high-temperature perovskite ferromagnetic insulator".  United States.  doi:10.1073/pnas.1707817115.  https://www.osti.gov/servlets/purl/1465448.

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@article{osti_1465448,

  title        = {Strain-induced high-temperature perovskite ferromagnetic insulator},

  author       = {Meng, Dechao and Guo, Hongli and Cui, Zhangzhang and Ma, Chao and Zhao, Jin and Lu, Jiangbo and Xu, Hui and Wang, Zhicheng and Hu, Xiang and Fu, Zhengping and Peng, Ranran and Guo, Jinghua and Zhai, Xiaofang and Brown, Gail J. and Knize, Randy and Lu, Yalin},

  abstractNote = {Ferromagnetic insulators are required for many new magnetic devices, such as dissipationless quantum-spintronic devices, magnetic tunneling junctions, etc. Ferromagnetic insulators with a high Curie temperature and a high-symmetry structure are critical integration with common single-crystalline oxide films or substrates. So far, the commonly used ferromagnetic insulators mostly possess low-symmetry structures associated with a poor growth quality and widespread properties. The few known high-symmetry materials either have extremely low Curie temperatures (≤16 K), or require chemical doping of an otherwise antiferromagnetic matrix. Here we present compelling evidence that the LaCoO3 single-crystalline thin film under tensile strain is a rare undoped perovskite ferromagnetic insulator with a remarkably high TC of up to 90 K. Both experiments and first-principles calculations demonstrate tensile-strain-induced ferromagnetism which does not exist in bulk LaCoO3. The ferromagnetism is strongest within a nearly stoichiometric structure, disappearing when the Co2+ defect concentration reaches about 10%. Furthermore, significant impact of the research includes demonstration of a strain-induced high-temperature ferromagnetic insulator, successful elevation of the transition over the liquid-nitrogen temperature, and high potential for integration into large-area device fabrication processes.},

  doi          = {10.1073/pnas.1707817115},

  journal      = {Proceedings of the National Academy of Sciences of the United States of America},

  number       = 12,

  volume       = 115,

  place        = {United States},

  year         = {2018},

  month        = {3}

}

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DOI: 10.1073/pnas.1707817115

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Title: Strain-induced high-temperature perovskite ferromagnetic insulator

Abstract

Citation Formats

Considerations on Double Exchange journal, October 1955

Coexistence of Low Damping and Strong Magnetoelastic Coupling in Epitaxial Spinel Ferrite Thin Films journal, July 2017

Multiplet effects in X-ray spectroscopy journal, January 2005

Spin State Transition in LaCoO 3 Studied Using Soft X-ray Absorption Spectroscopy and Magnetic Circular Dichroism journal, October 2006

Exchange Coupling in Eu Monochalcogenides from First Principles journal, May 2005

Ferromagnetism enhanced by structural relaxation of biaxially compressed LaCoO 3 films journal, April 2011

The magnetic, optical, and transport properties of representatives of a class of magnetic semiconductors: The europium chalcogenides journal, August 1986

Room-Temperature Ferromagnetism in Transparent Transition Metal-Doped Titanium Dioxide journal, January 2001

Insulating Ferromagnetic LaCoO 3 − δ Films: A Phase Induced by Ordering of Oxygen Vacancies journal, February 2014

X-ray absorption and magnetic circular dichroism of LaCoO 3 , La 0.7 Ce 0.3 CoO 3 , and La 0.7 Sr 0.3 CoO 3 films: Evidence for cobalt-valence-dependent magnetism journal, November 2010

A strong ferroelectric ferromagnet created by means of spin–lattice coupling journal, August 2010

Antiferromagnetism. Theory of Superexchange Interaction journal, July 1950

Intermediate-spin state and properties of LaCoO 3 journal, August 1996

Interaction Between the d Shells in the Transition Metals journal, February 1951

2 p x-ray absorption of 3 d transition-metal compounds: An atomic multiplet description including the crystal field journal, September 1990

Strain-driven spin-state transition and superexchange interaction in LaCoO 3 : A b initio study journal, July 2012

Suppression of spin-state transition in epitaxially strained LaCoO 3 journal, November 2008

Charge Ordering Induced Ferromagnetic Insulator: K 2 Cr 8 O 16 journal, June 2010

Effects of Double Exchange in Magnetic Crystals journal, April 1960

Indirect Exchange Coupling of Nuclear Magnetic Moments by Conduction Electrons journal, October 1954

An interpretation of the magnetic properties of the perovskite-type mixed crystals La1−xSrxCoO3−λ journal, August 1958

Superexchange interaction and symmetry properties of electron orbitals journal, July 1959

Making Nonmagnetic Semiconductors Ferromagnetic journal, August 1998

Matrix-Mediated Synthesis of Nanocrystalline ggr-Fe2O3: A New Optically Transparent Magnetic Material journal, July 1992

Ferromagnetic insulating state in tensile-strained LaCoO 3 thin films from LDA + U calculations journal, April 2012

A high-temperature ferromagnetic topological insulating phase by proximity coupling journal, May 2016

Long-range ferromagnetic order in LaCoO 3 − δ epitaxial films due to the interplay of epitaxial strain and oxygen vacancy ordering journal, April 2015

Ferromagnetic order in epitaxially strained La Co O 3 thin films journal, April 2007

Ferromagnetic Europium Compounds journal, March 1964

Strain-Induced Spin States in Atomically Ordered Cobaltites journal, January 2012

Three-Dimensional Magnetic Correlations in Multiferroic LuFe 2 O 4 journal, March 2008

Ferromagnetic spin-correlations in strained LaCoO3 thin films journal, November 2008

Low Temperature Magnetoresistance and the Magnetic Phase Diagram of La 1 − x Ca x MnO 3 journal, October 1995

X-ray absorption near-edge spectroscopy study of Mn and Co valence states in LaMn 1 − x Co x O 3 ( x = 0 – 1 ) journal, March 2006

Controlling the Magnetic Properties of LaMnO 3 /SrTiO 3 Heterostructures by Stoichiometry and Electronic Reconstruction: Atomic‐Scale Evidence journal, May 2019

Interface Engineered Room‐Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films journal, November 2019

Realization of Monophased LaCoO x Films with Ordered Oxygen Vacancies journal, December 2019

Co 2+ substituted La 2 CuO 4 /LaCoO 3 perovskite nanocomposites: synthesis, properties and heterogeneous catalytic performance journal, January 2018

Proximity-induced magnetism and an anomalous Hall effect in Bi 2 Se 3 /LaCoO 3 : a topological insulator/ferromagnetic insulator thin film heterostructure journal, January 2018

Seeking large Seebeck effects in LaX(X = Mn and Co)O 3 /SrTiO 3 superlattices by exploiting high spin-polarized effects journal, January 2019

Rare-earth-containing perovskite nanomaterials: design, synthesis, properties and applications journal, January 2020

High throughput study on magnetic ground states with Hubbard U corrections in transition metal dihalide monolayers journal, January 2020

High-temperature ferromagnetic insulating phase in strained La 0.8 Sr 0.2 MnO 3 thin films journal, September 2019

Strain effects on conductivity and charge transport in La-doped BaTiO 3 thin films journal, December 2019

Topotactic transition between perovskite and brownmillerite phases for epitaxial LaCoO 3− δ films and effects thus resulted journal, February 2020

Weak ferromagnetic insulator with huge coercivity in monoclinic double perovskite La 2 CuIrO 6 journal, July 2019

Hydrostatic pressure induced structural phase transition and mechanical properties of fluoroperovskite journal, October 2019

( LaCo O 3 ) n / ( SrCo O 2.5 ) n superlattices: Tunable ferromagnetic insulator journal, August 2019

Perpendicular magnetic anisotropy in L a 1 − x S r x Co O 2.5 + δ / L a 2 / 3 S r 1 / 3 Mn O 3 / L a 1 − x S r x Co O 2.5 + δ trilayers ( x = 0.05 – 0.5 ) journal, September 2019

Low-energy orbital excitations in strained LaCoO 3 films journal, October 2019

Exploring the structural, electronic, and magnetic properties of cation-ordered 3 d − 5 d double-perovskite Bi 2 FeReO 6 and Bi 2 FeIrO 6 thin films from first principles journal, December 2019

Exchange-biased nanocomposite ferromagnetic insulator journal, January 2020

Self-consistent site-dependent DFT+ U study of stoichiometric and defective SrMnO 3 journal, March 2019

Emergence of a Multiferroic Half-Metallic Phase in Bi 2 FeCrO 6 through Interplay of Hole Doping and Epitaxial Strain journal, September 2019

Direct imaging revealing halved ferromagnetism in tensile-strained LaCo O 3 thin films journal, July 2019

Maximization of ferromagnetism in LaCo O 3 films by competing symmetry journal, November 2019

Considerations on Double Exchange
journal, October 1955

Coexistence of Low Damping and Strong Magnetoelastic Coupling in Epitaxial Spinel Ferrite Thin Films
journal, July 2017

Multiplet effects in X-ray spectroscopy
journal, January 2005

Spin State Transition in ${LaCoO}_{3}$ Studied Using Soft X-ray Absorption Spectroscopy and Magnetic Circular Dichroism
journal, October 2006

Exchange Coupling in Eu Monochalcogenides from First Principles
journal, May 2005

Ferromagnetism enhanced by structural relaxation of biaxially compressed LaCoO ₃ films
journal, April 2011

The magnetic, optical, and transport properties of representatives of a class of magnetic semiconductors: The europium chalcogenides
journal, August 1986

Room-Temperature Ferromagnetism in Transparent Transition Metal-Doped Titanium Dioxide
journal, January 2001

Insulating Ferromagnetic ${LaCoO}_{3 - δ}$ Films: A Phase Induced by Ordering of Oxygen Vacancies
journal, February 2014

X-ray absorption and magnetic circular dichroism of ${LaCoO}_{3}$ , ${La}_{0.7} {Ce}_{0.3} {CoO}_{3}$ , and ${La}_{0.7} {Sr}_{0.3} {CoO}_{3}$ films: Evidence for cobalt-valence-dependent magnetism
journal, November 2010

A strong ferroelectric ferromagnet created by means of spin–lattice coupling
journal, August 2010

Antiferromagnetism. Theory of Superexchange Interaction
journal, July 1950

Intermediate-spin state and properties of ${LaCoO}_{3}$
journal, August 1996

Interaction Between the $d$ Shells in the Transition Metals
journal, February 1951

2 p x-ray absorption of 3 d transition-metal compounds: An atomic multiplet description including the crystal field
journal, September 1990

Strain-driven spin-state transition and superexchange interaction in LaCoO $_{3}$ : $A b$ initio study
journal, July 2012

Suppression of spin-state transition in epitaxially strained ${LaCoO}_{3}$
journal, November 2008

Charge Ordering Induced Ferromagnetic Insulator: $K_{2} {Cr}_{8} O_{16}$
journal, June 2010

Effects of Double Exchange in Magnetic Crystals
journal, April 1960

Indirect Exchange Coupling of Nuclear Magnetic Moments by Conduction Electrons
journal, October 1954

An interpretation of the magnetic properties of the perovskite-type mixed crystals La1−xSrxCoO3−λ
journal, August 1958

Superexchange interaction and symmetry properties of electron orbitals
journal, July 1959

Making Nonmagnetic Semiconductors Ferromagnetic
journal, August 1998

Matrix-Mediated Synthesis of Nanocrystalline ggr-Fe2O3: A New Optically Transparent Magnetic Material
journal, July 1992

Ferromagnetic insulating state in tensile-strained LaCoO $_{3}$ thin films from LDA $+$ $U$ calculations
journal, April 2012

A high-temperature ferromagnetic topological insulating phase by proximity coupling
journal, May 2016

Long-range ferromagnetic order in ${LaCoO}_{3 - δ}$ epitaxial films due to the interplay of epitaxial strain and oxygen vacancy ordering
journal, April 2015

Ferromagnetic order in epitaxially strained $La Co O_{3}$ thin films
journal, April 2007

Ferromagnetic Europium Compounds
journal, March 1964

Strain-Induced Spin States in Atomically Ordered Cobaltites
journal, January 2012

Three-Dimensional Magnetic Correlations in Multiferroic ${LuFe}_{2} O_{4}$
journal, March 2008

Ferromagnetic spin-correlations in strained LaCoO3 thin films
journal, November 2008

Low Temperature Magnetoresistance and the Magnetic Phase Diagram of ${La}_{1 - x} {Ca}_{x} {MnO}_{3}$
journal, October 1995

X-ray absorption near-edge spectroscopy study of Mn and Co valence states in ${LaMn}_{1 - x} {Co}_{x} O_{3} (x = 0 - 1)$
journal, March 2006

Controlling the Magnetic Properties of LaMnO ₃ /SrTiO ₃ Heterostructures by Stoichiometry and Electronic Reconstruction: Atomic‐Scale Evidence
journal, May 2019

Interface Engineered Room‐Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films
journal, November 2019

Realization of Monophased LaCoO _x Films with Ordered Oxygen Vacancies
journal, December 2019

Co ²⁺ substituted La ₂ CuO ₄ /LaCoO ₃ perovskite nanocomposites: synthesis, properties and heterogeneous catalytic performance
journal, January 2018

Proximity-induced magnetism and an anomalous Hall effect in Bi ₂ Se ₃ /LaCoO ₃ : a topological insulator/ferromagnetic insulator thin film heterostructure
journal, January 2018

Seeking large Seebeck effects in LaX(X = Mn and Co)O ₃ /SrTiO ₃ superlattices by exploiting high spin-polarized effects
journal, January 2019

Rare-earth-containing perovskite nanomaterials: design, synthesis, properties and applications
journal, January 2020

High throughput study on magnetic ground states with Hubbard U corrections in transition metal dihalide monolayers
journal, January 2020

High-temperature ferromagnetic insulating phase in strained La _0.8 Sr _0.2 MnO ₃ thin films
journal, September 2019

Strain effects on conductivity and charge transport in La-doped BaTiO ₃ thin films
journal, December 2019

Topotactic transition between perovskite and brownmillerite phases for epitaxial LaCoO _{3− δ} films and effects thus resulted
journal, February 2020

Weak ferromagnetic insulator with huge coercivity in monoclinic double perovskite La ₂ CuIrO ₆
journal, July 2019

Hydrostatic pressure induced structural phase transition and mechanical properties of fluoroperovskite
journal, October 2019

${(LaCo O_{3})}_{n} / {(SrCo O_{2.5})}_{n}$ superlattices: Tunable ferromagnetic insulator
journal, August 2019

Perpendicular magnetic anisotropy in $L a_{1 - x} S r_{x} Co O_{2.5 + δ} / L a_{2 / 3} S r_{1 / 3} Mn O_{3} / L a_{1 - x} S r_{x} Co O_{2.5 + δ}$ trilayers $(x = 0.05 - 0.5)$
journal, September 2019

Low-energy orbital excitations in strained ${LaCoO}_{3}$ films
journal, October 2019

Exploring the structural, electronic, and magnetic properties of cation-ordered $3 d − 5 d$ double-perovskite ${Bi}_{2} {FeReO}_{6}$ and ${Bi}_{2} {FeIrO}_{6}$ thin films from first principles
journal, December 2019

Exchange-biased nanocomposite ferromagnetic insulator
journal, January 2020

Self-consistent site-dependent DFT+ $U$ study of stoichiometric and defective ${SrMnO}_{3}$
journal, March 2019

Emergence of a Multiferroic Half-Metallic Phase in ${Bi}_{2} {FeCrO}_{6}$ through Interplay of Hole Doping and Epitaxial Strain
journal, September 2019

Direct imaging revealing halved ferromagnetism in tensile-strained $LaCo O_{3}$ thin films
journal, July 2019

Maximization of ferromagnetism in $LaCo O_{3}$ films by competing symmetry
journal, November 2019