Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped BiFeO3

Morozovska, Anna N.; Eliseev, Eugene A.; Chen, Deyang; Nelson, Christopher T.; Kalinin, Sergei V.

doi:10.1103/PhysRevB.99.195440

Title: Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped $BiFe O_{3}$

Abstract

Scanning transmission electron microscopy (STEM) has enabled mapping of atomic structures of solids with sub-picometer precision, providing insight to the physics of ferroic phenomena and chemical expansion. Yet, only a subset of information is available, due to projective nature of imaging in the beam direction. Correspondingly, the analysis often relies on the postulated form of macroscopic Landau-Ginzburg energy for the ferroic long-range order parameter, and some predefined relationship between experimentally determined atomic coordinates and the order-parameter field. Here, we propose an approach for exploring the structure of ferroics using reduced order-parameter models constructed based on experimental data only. We develop a four-sublattice model (FSM) for the analytical description of A-cation displacement in (anti)ferroelectric-antiferrodistortive perovskites of ABO₃ type. The model describes the displacements of cation A in four neighboring unit cells and determines the conditions of different structural phases’ appearance and stability in ABO₃. We show that FSM explains the coexistence of rhombohedral, orthorhombic, and spatially modulated phases, observed by atomic-resolution STEM in La-doped BiFeO₃. Using this method, we atomically resolve and theoretically model the sublattice asymmetry inherent to the case of the A-site La/Bi cation sublattice in La_xBi_1-xFeO₃ polymorphs. This approach allows the exploration of ferroic behaviors from experimental datamore »« less

Authors:

Morozovska, Anna N. ^[1]; Eliseev, Eugene A. ^[2]; Chen, Deyang ^[3];

^[4];

^[4]

NAS of Ukraine, Kyiv (Ukraine). Inst. of Physics
NAS of Ukraine, Kyiv (Ukraine). Inst. of Problems for Material Sciences
South China Normal Univ., Guangzhou (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Wed May 22 00:00:00 EDT 2019

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC); National Academy of Sciences of Ukraine

OSTI Identifier:: 1530059

Alternate Identifier(s):: OSTI ID: 1515098

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 99; Journal Issue: 19; 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

Citation Formats


                    Morozovska, Anna N., Eliseev, Eugene A., Chen, Deyang, Nelson, Christopher T., and Kalinin, Sergei V. Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped BiFeO3.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevB.99.195440.

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                    Morozovska, Anna N., Eliseev, Eugene A., Chen, Deyang, Nelson, Christopher T., & Kalinin, Sergei V. Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped BiFeO3.  United States.  https://doi.org/10.1103/PhysRevB.99.195440

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                    Morozovska, Anna N., Eliseev, Eugene A., Chen, Deyang, Nelson, Christopher T., and Kalinin, Sergei V. Wed .  
"Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped BiFeO3".  United States.  https://doi.org/10.1103/PhysRevB.99.195440.  https://www.osti.gov/servlets/purl/1530059.

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@article{osti_1530059,

  title        = {Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped BiFeO3},

  author       = {Morozovska, Anna N. and Eliseev, Eugene A. and Chen, Deyang and Nelson, Christopher T. and Kalinin, Sergei V.},

  abstractNote = {Scanning transmission electron microscopy (STEM) has enabled mapping of atomic structures of solids with sub-picometer precision, providing insight to the physics of ferroic phenomena and chemical expansion. Yet, only a subset of information is available, due to projective nature of imaging in the beam direction. Correspondingly, the analysis often relies on the postulated form of macroscopic Landau-Ginzburg energy for the ferroic long-range order parameter, and some predefined relationship between experimentally determined atomic coordinates and the order-parameter field. Here, we propose an approach for exploring the structure of ferroics using reduced order-parameter models constructed based on experimental data only. We develop a four-sublattice model (FSM) for the analytical description of A-cation displacement in (anti)ferroelectric-antiferrodistortive perovskites of ABO3 type. The model describes the displacements of cation A in four neighboring unit cells and determines the conditions of different structural phases’ appearance and stability in ABO3. We show that FSM explains the coexistence of rhombohedral, orthorhombic, and spatially modulated phases, observed by atomic-resolution STEM in La-doped BiFeO3. Using this method, we atomically resolve and theoretically model the sublattice asymmetry inherent to the case of the A-site La/Bi cation sublattice in LaxBi1-xFeO3 polymorphs. This approach allows the exploration of ferroic behaviors from experimental data only, without additional assumptions on the nature of the order parameter.},

  doi          = {10.1103/PhysRevB.99.195440},

  journal      = {Physical Review B},

  number       = 19,

  volume       = 99,

  place        = {United States},

  year         = {Wed May 22 00:00:00 EDT 2019},

  month        = {Wed May 22 00:00:00 EDT 2019}

}

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Title: Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped BiFe O 3

Abstract

Citation Formats

Slush-like polar structures in single-crystal relaxors journal, June 2017

Ferroelectricity in Ultrathin Perovskite Films journal, June 2004

Observation of polar vortices in oxide superlattices journal, January 2016

Domain Dynamics During Ferroelectric Switching journal, November 2011

Scanning force microscopy for the study of domain structure in ferroelectric thin films journal, March 1996

Mechanical Writing of Ferroelectric Polarization journal, April 2012

XCVI. Theory of barium titanate: Part I journal, October 1949

Phase-Field Method of Phase Transitions/Domain Structures in Ferroelectric Thin Films: A Review journal, June 2008

Quantification of flexoelectricity in PbTiO3/SrTiO3 superlattice polar vortices using machine learning and phase-field modeling journal, November 2017

Unit-cell scale mapping of ferroelectricity and tetragonality in epitaxial ultrathin ferroelectric films journal, December 2006

Spatially resolved steady-state negative capacitance journal, January 2019

Spontaneous Vortex Nanodomain Arrays at Ferroelectric Heterointerfaces journal, February 2011

Diffraction contrast analysis of 90° and 180° ferroelectric domain structures of PbTiO 3 thin films journal, June 2011

Epitaxial BiFeO3 Multiferroic Thin Film Heterostructures journal, March 2003

Temperature dependence of the crystal and magnetic structures of BiFeO 3 journal, April 1980

Structure of a ferroelectric and ferroelastic monodomain crystal of the perovskite BiFeO3 journal, December 1990

A Strain-Driven Morphotropic Phase Boundary in BiFeO3 journal, November 2009

Evidence for Room-Temperature Multiferroicity in a Compound with a Giant Axial Ratio journal, May 2009

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High Pressure Crystal and Magnetic Phase Transitions in Multiferroic Bi 0.9 La 0.1 FeO 3 journal, December 2013

Combinatorial discovery of a lead-free morphotropic phase boundary in a thin-film piezoelectric perovskite journal, May 2008

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Universal Behavior and Electric-Field-Induced Structural Transition in Rare-Earth-Substituted BiFeO3 journal, March 2010

Structural transitions and complex domain structures across a ferroelectric-to-antiferroelectric phase boundary in epitaxial Sm-doped BiFeO 3 thin films journal, July 2009

Picometer-scale atom position analysis in annular bright-field STEM imaging journal, January 2018

A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics journal, January 1958

Title: Building a free-energy functional from atomically resolved imaging: Atomic-scale phenomena in La-doped $BiFe O_{3}$

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journal, June 2017

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journal, June 2004

Observation of polar vortices in oxide superlattices
journal, January 2016

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journal, March 1996

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XCVI. Theory of barium titanate: Part I
journal, October 1949

Phase-Field Method of Phase Transitions/Domain Structures in Ferroelectric Thin Films: A Review
journal, June 2008

Quantification of flexoelectricity in PbTiO3/SrTiO3 superlattice polar vortices using machine learning and phase-field modeling
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Unit-cell scale mapping of ferroelectricity and tetragonality in epitaxial ultrathin ferroelectric films
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Spatially resolved steady-state negative capacitance
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Spontaneous Vortex Nanodomain Arrays at Ferroelectric Heterointerfaces
journal, February 2011

Diffraction contrast analysis of 90° and 180° ferroelectric domain structures of PbTiO ₃ thin films
journal, June 2011

Epitaxial BiFeO₃ Multiferroic Thin Film Heterostructures
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Temperature dependence of the crystal and magnetic structures of BiFeO ₃
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Structure of a ferroelectric and ferroelastic monodomain crystal of the perovskite BiFeO3
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A Strain-Driven Morphotropic Phase Boundary in BiFeO₃
journal, November 2009

Evidence for Room-Temperature Multiferroicity in a Compound with a Giant Axial Ratio
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High Pressure Crystal and Magnetic Phase Transitions in Multiferroic Bi _0.9 La _0.1 FeO ₃
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Combinatorial discovery of a lead-free morphotropic phase boundary in a thin-film piezoelectric perovskite
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Universal Behavior and Electric-Field-Induced Structural Transition in Rare-Earth-Substituted BiFeO3
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Structural transitions and complex domain structures across a ferroelectric-to-antiferroelectric phase boundary in epitaxial Sm-doped ${BiFeO}_{3}$ thin films
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Picometer-scale atom position analysis in annular bright-field STEM imaging
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A thermodynamic theory of “weak” ferromagnetism of antiferromagnetics
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