Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure

Guo, Er-Jia; Desautels, Ryan; Lee, Dongkyu; Roldan, Manuel A.; Liao, Zhaoliang; Charlton, Timothy; Ambaye, Haile; Molaison, Jamie; Boehler, Reinhard; Keavney, David; Herklotz, Andreas; Ward, T. Zac; Lee, Ho Nyung; Fitzsimmons, Michael R.

doi:10.1103/PhysRevLett.122.187202

Title: Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure

Abstract

In the bulk, LaCoO₃ (LCO) is a paramagnet, yet the low-temperature ferromagnetism (FM) is observed in tensile strained thin films, and its origin remains unresolved. Here, we quantitatively measured the distribution of atomic density and magnetization in LCO films by polarized neutron reflectometry (PNR) and found that the LCO layers near the heterointerfaces exhibit a reduced magnetization but an enhanced atomic density, whereas the film’s interior (i.e., its film bulk) shows the opposite trend. We attribute the nonuniformity to the symmetry mismatch at the interface, which induces a structural distortion related to the ferroelasticity of LCO. This assertion is tested by systematic application of hydrostatic pressure during the PNR experiments. The magnetization can be controlled at a rate of -20.4% per GPa. These results provide unique insights into mechanisms driving FM in strained LCO films while offering a tantalizing observation that tunable deformation of the CoO₆ octahedra in combination with the ferroelastic order parameter.

Authors:

Guo, Er-Jia ^[1]; Desautels, Ryan ^[2]; Lee, Dongkyu ^[2]; Roldan, Manuel A. ^[3]; Liao, Zhaoliang ^[2]; Charlton, Timothy ^[2]; Ambaye, Haile ^[2]; Molaison, Jamie ^[2]; Boehler, Reinhard ^[4]; Keavney, David ^[5]; Herklotz, Andreas ^[6]; Ward, T. Zac ^[2]; Lee, Ho Nyung ^[2]; Fitzsimmons, Michael R. ^[7]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China); Univ. of Chinese Academy of Sciences, Beijing (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Arizona State Univ., Tempe, AZ (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Carnegie Inst. of Science, Washington, D.C. (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Martin-Luther-Univ. Halle-Wittenberg, Halle (Saale) (Germany)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:: Wed May 08 00:00:00 EDT 2019

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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

OSTI Identifier:: 1542188

Alternate Identifier(s):: OSTI ID: 1511519; OSTI ID: 1561629

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

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Letters

Additional Journal Information:: Journal Volume: 122; Journal Issue: 18; Journal ID: ISSN 0031-9007

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; ferroelastic materials; hydrostatic pressure; polarized neutron reflectometry; spin state transition; x-ray absorption

Citation Formats


                    Guo, Er-Jia, Desautels, Ryan, Lee, Dongkyu, Roldan, Manuel A., Liao, Zhaoliang, Charlton, Timothy, Ambaye, Haile, Molaison, Jamie, Boehler, Reinhard, Keavney, David, Herklotz, Andreas, Ward, T. Zac, Lee, Ho Nyung, and Fitzsimmons, Michael R. Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevLett.122.187202.

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                    Guo, Er-Jia, Desautels, Ryan, Lee, Dongkyu, Roldan, Manuel A., Liao, Zhaoliang, Charlton, Timothy, Ambaye, Haile, Molaison, Jamie, Boehler, Reinhard, Keavney, David, Herklotz, Andreas, Ward, T. Zac, Lee, Ho Nyung, & Fitzsimmons, Michael R. Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure.  United States.  https://doi.org/10.1103/PhysRevLett.122.187202

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                    Guo, Er-Jia, Desautels, Ryan, Lee, Dongkyu, Roldan, Manuel A., Liao, Zhaoliang, Charlton, Timothy, Ambaye, Haile, Molaison, Jamie, Boehler, Reinhard, Keavney, David, Herklotz, Andreas, Ward, T. Zac, Lee, Ho Nyung, and Fitzsimmons, Michael R. Wed .  
"Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure".  United States.  https://doi.org/10.1103/PhysRevLett.122.187202.  https://www.osti.gov/servlets/purl/1542188.

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@article{osti_1542188,

  title        = {Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure},

  author       = {Guo, Er-Jia and Desautels, Ryan and Lee, Dongkyu and Roldan, Manuel A. and Liao, Zhaoliang and Charlton, Timothy and Ambaye, Haile and Molaison, Jamie and Boehler, Reinhard and Keavney, David and Herklotz, Andreas and Ward, T. Zac and Lee, Ho Nyung and Fitzsimmons, Michael R.},

  abstractNote = {In the bulk, LaCoO3 (LCO) is a paramagnet, yet the low-temperature ferromagnetism (FM) is observed in tensile strained thin films, and its origin remains unresolved. Here, we quantitatively measured the distribution of atomic density and magnetization in LCO films by polarized neutron reflectometry (PNR) and found that the LCO layers near the heterointerfaces exhibit a reduced magnetization but an enhanced atomic density, whereas the film’s interior (i.e., its film bulk) shows the opposite trend. We attribute the nonuniformity to the symmetry mismatch at the interface, which induces a structural distortion related to the ferroelasticity of LCO. This assertion is tested by systematic application of hydrostatic pressure during the PNR experiments. The magnetization can be controlled at a rate of -20.4% per GPa. These results provide unique insights into mechanisms driving FM in strained LCO films while offering a tantalizing observation that tunable deformation of the CoO6 octahedra in combination with the ferroelastic order parameter.},

  doi          = {10.1103/PhysRevLett.122.187202},

  journal      = {Physical Review Letters},

  number       = 18,

  volume       = 122,

  place        = {United States},

  year         = {Wed May 08 00:00:00 EDT 2019},

  month        = {Wed May 08 00:00:00 EDT 2019}

}

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Works referenced in this record:

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Works referencing / citing this record:

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

Li, Sisi; Wang, Jiesu; Zhang, Qinghua
Physical Review Materials, Vol. 3, Issue 11
DOI: 10.1103/physrevmaterials.3.114409

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Title: Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure

Abstract

Citation Formats

Temperature- and pressure-induced spin-state transitions in LaCoO 3 journal, January 2006

Elastic properties of SrTiO 3 crystals at ultralow frequencies journal, June 1999

The atomic structure of the Σ = 13(θ = 22.6°)[001] twist boundary in gold determined using quantitative X-ray diffraction techniques journal, April 1989

Strain-driven magnetism in LaCoO 3 thin films journal, January 2009

Switchable orbital polarization and magnetization in strained LaCo O 3 films journal, January 2019

Ferroelasticity and spin-state transitions of LaCoO 3 journal, July 2014

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

Temperature- and pressure-driven spin-state transitions in LaCoO 3 journal, February 2007

Magnetic and electrical anomalies in LaCoO3 journal, August 1964

Bistable Magnetism and Potential for Voltage-Induced Spin Crossover in Dilute Magnetic Ferroelectrics journal, June 2015

First-Order Localized-Electron ⇆ Collective-Electron Transition in LaCo O 3 journal, March 1967

Structural and thermoelectric characterization of Ba substituted LaCoO3 perovskite-type materials obtained by polymerized gel combustion method journal, December 2013

Spin-State Transition in LaCoO 3 : Direct Neutron Spectroscopic Evidence of Excited Magnetic States journal, December 2006

EosFit7c and a Fortran module (library) for equation of state calculations journal, January 2014

Nanoscale Spin-State Ordering in LaCoO 3 Epitaxial Thin Films journal, April 2014

Tuning the magnetism of epitaxial cobalt oxide thin films by electron beam irradiation journal, July 2017

Local lattice distortion during the spin-state transition in LaCoO 3 journal, April 1997

Reversible strain effect on the magnetization of LaCoO 3 films journal, March 2009

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

Tuning the magnetic properties of La Co O 3 thin films by epitaxial strain journal, January 2008

Bulk modulus anomaly in R Co O 3 ( R = La , Pr, and Nd) journal, June 2005

Evidence for the excited triplet of Co 3 + in LaCoO 3 journal, September 2002

Direct Measurement of the Low-Temperature Spin-State Transition in LaCoO 3 journal, July 2007

In-situ neutron diffraction of LaCoO 3 perovskite under uniaxial compression. II. Elastic properties journal, July 2014

In Situ Observation of Oxygen Vacancy Dynamics and Ordering in the Epitaxial LaCoO 3 System journal, June 2017

Magnetism and phase transitions in LaCoO 3 journal, August 2013

Thermal and mechanical properties of LaCoO3 and La0.8Ca0.2CoO3 perovskites journal, July 2008

Pressure-induced intermediate-to-low spin state transition in LaCoO 3 journal, April 2003

Evidence for orbital ordering in LaCoO 3 journal, June 2003

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

Ferromagnetism in La Co O 3 journal, July 2004

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

Ferromagnetism in La Co O 3 nanoparticles journal, November 2007

Electric-field control of tri-state phase transformation with a selective dual-ion switch journal, May 2017

Size- and pressure-controlled ferromagnetism in LaCoO 3 nanoparticles journal, June 2008

Structural phenomena associated with the spin-state transition in LaCoO 3 journal, September 2002

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

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

Pressure Dependence of the 100 K Spin-State Transition in LaCoO 3 journal, April 1997

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

Temperature- and pressure-induced spin-state transitions in ${LaCoO}_{3}$
journal, January 2006

Elastic properties of SrTiO ₃ crystals at ultralow frequencies
journal, June 1999

The atomic structure of the Σ = 13(θ = 22.6°)[001] twist boundary in gold determined using quantitative X-ray diffraction techniques
journal, April 1989

Strain-driven magnetism in ${LaCoO}_{3}$ thin films
journal, January 2009

Switchable orbital polarization and magnetization in strained $LaCo O_{3}$ films
journal, January 2019

Ferroelasticity and spin-state transitions of LaCoO ₃
journal, July 2014

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

Temperature- and pressure-driven spin-state transitions in ${LaCoO}_{3}$
journal, February 2007

Magnetic and electrical anomalies in LaCoO3
journal, August 1964

Bistable Magnetism and Potential for Voltage-Induced Spin Crossover in Dilute Magnetic Ferroelectrics
journal, June 2015

First-Order Localized-Electron $⇆$ Collective-Electron Transition in LaCo $O_{3}$
journal, March 1967

Structural and thermoelectric characterization of Ba substituted LaCoO3 perovskite-type materials obtained by polymerized gel combustion method
journal, December 2013

Spin-State Transition in ${LaCoO}_{3}$ : Direct Neutron Spectroscopic Evidence of Excited Magnetic States
journal, December 2006

EosFit7c and a Fortran module (library) for equation of state calculations
journal, January 2014

Nanoscale Spin-State Ordering in LaCoO ₃ Epitaxial Thin Films
journal, April 2014

Tuning the magnetism of epitaxial cobalt oxide thin films by electron beam irradiation
journal, July 2017

Local lattice distortion during the spin-state transition in ${LaCoO}_{3}$
journal, April 1997

Reversible strain effect on the magnetization of ${LaCoO}_{3}$ films
journal, March 2009

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

Tuning the magnetic properties of $La Co O_{3}$ thin films by epitaxial strain
journal, January 2008

Bulk modulus anomaly in $R Co O_{3}$ ( $R = La$ , Pr, and Nd)
journal, June 2005

Evidence for the excited triplet of ${Co}^{3 +}$ in ${LaCoO}_{3}$
journal, September 2002

Direct Measurement of the Low-Temperature Spin-State Transition in ${LaCoO}_{3}$
journal, July 2007

In-situ neutron diffraction of LaCoO ₃ perovskite under uniaxial compression. II. Elastic properties
journal, July 2014

In Situ Observation of Oxygen Vacancy Dynamics and Ordering in the Epitaxial LaCoO ₃ System
journal, June 2017

Magnetism and phase transitions in LaCoO ₃
journal, August 2013

Thermal and mechanical properties of LaCoO3 and La0.8Ca0.2CoO3 perovskites
journal, July 2008

Pressure-induced intermediate-to-low spin state transition in ${LaCoO}_{3}$
journal, April 2003

Evidence for orbital ordering in ${LaCoO}_{3}$
journal, June 2003

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

Ferromagnetism in $La Co O_{3}$
journal, July 2004

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

Ferromagnetism in $La Co O_{3}$ nanoparticles
journal, November 2007

Electric-field control of tri-state phase transformation with a selective dual-ion switch
journal, May 2017

Size- and pressure-controlled ferromagnetism in ${LaCoO}_{3}$ nanoparticles
journal, June 2008

Structural phenomena associated with the spin-state transition in ${LaCoO}_{3}$
journal, September 2002

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

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

Pressure Dependence of the 100 K Spin-State Transition in LaCoO ₃
journal, April 1997

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