Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Kim, Jieun; Takenaka, Hiroyuki; Qi, Yubo; Damodaran, Anoop R.; Fernandez, Abel; Gao, Ran; McCarter, Margaret R.; Saremi, Sahar; Chung, Linh; Rappe, Andrew M.; Martin, Lane W.

doi:10.1002/adma.201901060

Title: Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Abstract

Understanding and ultimately controlling the large electromechanical effects in relaxor ferroelectrics requires intimate knowledge of how the local-polar order evolves under applied stimuli. Here, the biaxial-strain-induced evolution of and correlations between polar structures and properties in epitaxial films of the prototypical relaxor ferroelectric 0.68PbMg_1/3Nb_2/3O₃–0.32PbTiO₃ are investigated. X-ray diffuse-scattering studies reveal an evolution from a butterfly- to disc-shaped pattern and an increase in the correlation-length from ≈8 to ≈25 nm with increasing compressive strain. Molecular-dynamics simulations reveal the origin of the changes in the diffuse-scattering patterns and that strain induces polarization rotation and the merging of the polar order. As the magnitude of the strain is increased, relaxor behavior is gradually suppressed but is not fully quenched. Analysis of the dynamic evolution of dipole alignment in the simulations reveals that, while, for most unit-cell chemistries and configurations, strain drives a tendency toward more ferroelectric-like order, there are certain unit cells that become more disordered under strain, resulting in stronger competition between ordered and disordered regions and enhanced overall susceptibilities. Ultimately, this implies that deterministic creation of specific local chemical configurations could be an effective way to enhance relaxor performance.

Authors:

^[1]; Takenaka, Hiroyuki ^[2]; Qi, Yubo ^[3]; Damodaran, Anoop R. ^[1]; Fernandez, Abel ^[1]; Gao, Ran ^[1]; McCarter, Margaret R. ^[1]; Saremi, Sahar ^[1]; Chung, Linh ^[1]; Rappe, Andrew M. ^[3]; Martin, Lane W. ^[4]

Univ. of California, Berkeley, CA (United States)
Univ. of Nebraska, Lincoln, NE (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Publication Date:: Wed Apr 10 00:00:00 EDT 2019

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

Sponsoring Org.:: USDOE Office of Science (SC); US Department of the Navy, Office of Naval Research (ONR); US Army Research Office (ARO); National Science Foundation (NSF); Gordon and Betty Moore Foundation (GBMF); USDOD

OSTI Identifier:: 1633233

Alternate Identifier(s):: OSTI ID: 1506136

Grant/Contract Number:: AC02-05CH11231; FG02‐07ER46431; SC0012375; AC02‐06CH11357; N00014‐17‐1‐2574; W911NF‐14‐1‐0104; OISE‐1545907; DMR‐1719353; DMR‐1708615; GBMF5307; AC02‐05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Advanced Materials

Additional Journal Information:: Journal Volume: 31; Journal Issue: 21; Journal ID: ISSN 0935-9648

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; diffuse scattering; domain structure; polar nanodomains; relaxor ferroelectrics; strain control

Citation Formats


                    Kim, Jieun, Takenaka, Hiroyuki, Qi, Yubo, Damodaran, Anoop R., Fernandez, Abel, Gao, Ran, McCarter, Margaret R., Saremi, Sahar, Chung, Linh, Rappe, Andrew M., and Martin, Lane W. Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution.  United States: N. p., 2019. 
Web.  doi:10.1002/adma.201901060.

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                    Kim, Jieun, Takenaka, Hiroyuki, Qi, Yubo, Damodaran, Anoop R., Fernandez, Abel, Gao, Ran, McCarter, Margaret R., Saremi, Sahar, Chung, Linh, Rappe, Andrew M., & Martin, Lane W. Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution.  United States.  https://doi.org/10.1002/adma.201901060

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                    Kim, Jieun, Takenaka, Hiroyuki, Qi, Yubo, Damodaran, Anoop R., Fernandez, Abel, Gao, Ran, McCarter, Margaret R., Saremi, Sahar, Chung, Linh, Rappe, Andrew M., and Martin, Lane W. Wed .  
"Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution".  United States.  https://doi.org/10.1002/adma.201901060.  https://www.osti.gov/servlets/purl/1633233.

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@article{osti_1633233,

  title        = {Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution},

  author       = {Kim, Jieun and Takenaka, Hiroyuki and Qi, Yubo and Damodaran, Anoop R. and Fernandez, Abel and Gao, Ran and McCarter, Margaret R. and Saremi, Sahar and Chung, Linh and Rappe, Andrew M. and Martin, Lane W.},

  abstractNote = {Understanding and ultimately controlling the large electromechanical effects in relaxor ferroelectrics requires intimate knowledge of how the local-polar order evolves under applied stimuli. Here, the biaxial-strain-induced evolution of and correlations between polar structures and properties in epitaxial films of the prototypical relaxor ferroelectric 0.68PbMg1/3Nb2/3O3–0.32PbTiO3 are investigated. X-ray diffuse-scattering studies reveal an evolution from a butterfly- to disc-shaped pattern and an increase in the correlation-length from ≈8 to ≈25 nm with increasing compressive strain. Molecular-dynamics simulations reveal the origin of the changes in the diffuse-scattering patterns and that strain induces polarization rotation and the merging of the polar order. As the magnitude of the strain is increased, relaxor behavior is gradually suppressed but is not fully quenched. Analysis of the dynamic evolution of dipole alignment in the simulations reveals that, while, for most unit-cell chemistries and configurations, strain drives a tendency toward more ferroelectric-like order, there are certain unit cells that become more disordered under strain, resulting in stronger competition between ordered and disordered regions and enhanced overall susceptibilities. Ultimately, this implies that deterministic creation of specific local chemical configurations could be an effective way to enhance relaxor performance.},

  doi          = {10.1002/adma.201901060},

  journal      = {Advanced Materials},

  number       = 21,

  volume       = 31,

  place        = {United States},

  year         = {Wed Apr 10 00:00:00 EDT 2019},

  month        = {Wed Apr 10 00:00:00 EDT 2019}

}

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https://doi.org/10.1002/adma.201901060

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Cited by: 22 works

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Figures / Tables:

Figure 1: Characterization of crystal structure and diffuse-scattering. a) Wide-angle θ–2θ X-ray diffraction line scans of epitaxial 0.68Pb(Mg_1/3Nb_2/3) O₃–0.32PbTiO₃ (PMN-PT) thin films on various substrates. b) A zoom-in about the PMN-PT 002-diffraction condition. The ★ denotes peaks for the Ba_0.5Sr_0.5RuO₃ 002-diffraction condition and the dashed line denotes the position ofmore »

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Title: Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Abstract

Citation Formats

Figures / Tables:

The giant electromechanical response in ferroelectric relaxors as a critical phenomenon journal, June 2006

Intermediate temperature scale T ∗ in lead-based relaxor systems journal, August 2009

Crystalline ferroelectrics with glassy polarization behavior journal, September 1983

Ultrahigh piezoelectricity in ferroelectric ceramics by design journal, March 2018

Thin-film ferroelectric materials and their applications journal, November 2016

Tuning Susceptibility via Misfit Strain in Relaxed Morphotropic Phase Boundary PbZr 1-x Ti x O 3 Epitaxial Thin Films journal, May 2014

Pressure-Induced Suppression of the Diffuse Scattering in the Model Relaxor Ferroelectric P b M g 1 / 3 N b 2 / 3 O 3 journal, June 2003

Electric-field-induced redistribution of polar nano-regions in a relaxor ferroelectric journal, January 2006

Ultrahigh strain and piezoelectric behavior in relaxor based ferroelectric single crystals journal, August 1997

Ferroelectricity and Self-Polarization in Ultrathin Relaxor Ferroelectric Films journal, January 2016

X-ray and neutron diffraction investigations of the structural phase transformation sequence under electric field in 0.7Pb(Mg1∕3Nb2∕3)-0.3PbTiO3 crystal journal, August 2004

The relation of local order to material properties in relaxor ferroelectrics journal, June 2018

Properties of Epitaxial Films Made of Relaxor Ferroelectrics journal, December 2013

Diffuse X-Ray Scattering Study of Lead Magnesium Niobate Single Crystals journal, November 1997

Crystal Structure and Pair Potentials: A Molecular-Dynamics Study journal, October 1980

Three-dimensional mapping of diffuse scattering in Pb ( Zn 1 ∕ 3 Nb 2 ∕ 3 ) O 3 − x Pb Ti O 3 journal, November 2004

Relationship between Local Structure and Relaxor Behavior in Perovskite Oxides journal, December 2007

Relaxorferroelectrics: An overview journal, January 1994

Low-temperature relaxor state induced by epitaxial compression in PbSc 0.5 Nb 0.5 O 3 films journal, June 2013

Visualization of dielectric constant-electric field-temperature phase maps for imprinted relaxor ferroelectric thin films journal, March 2016

Diffuse scattering in relaxor ferroelectrics: true three-dimensional mapping, experimental artefacts and modelling journal, November 2011

Anisotropic Local Correlations and Dynamics in a Relaxor Ferroelectric journal, April 2013

Do we need the Ether of Polar Nanoregions? journal, April 2012

Perovskite phase stabilization in epitaxial Pb(Mg1/3Nb2/3)O3–PbTiO3 films by deposition onto vicinal (001) SrTiO3 substrates journal, November 2001

In-situ neutron diffraction study of Pb(In 1/2 Nb 1/2 )O 3 -Pb(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 single crystals under uniaxial mechanical stress journal, April 2012

Observation of Nanoscale 180 ° Stripe Domains in Ferroelectric P b T i O 3 Thin Films journal, July 2002

Effect of Mechanical Boundary Conditions on Phase Diagrams of Epitaxial Ferroelectric Thin Films journal, March 1998

Uniaxial-stress induced phase transitions in [001]C-poled 0.955Pb(Zn1∕3Nb2∕3)O3–0.045PbTiO3 journal, April 2007

Self-Accommodation of Ionic Size-Effect Atomic Displacements in Antiferroelectric Order in Relaxor Lead Scandium Niobate journal, May 1999

Phase instability induced by polar nanoregions in a relaxor ferroelectric system journal, May 2008

Relationship between local structure and phase transitions of a disordered solid solution journal, October 2002

Effect of mechanical constraint on the dielectric and piezoelectric behavior of epitaxial Pb(Mg1/3Nb2/3)O3(90%)–PbTiO3(10%) relaxor thin films journal, December 1999

Seeing the forest and the trees journal, June 2018

Neutron elastic diffuse scattering study of Pb ( Mg 1 / 3 Nb 2 / 3 ) O 3 journal, February 2004

Epitaxial Ferroelectric Heterostructures Fabricated by Selective Area Epitaxy of SrRuO3 Using an MgO Mask journal, February 2012

Pressure-Induced Crossover from Long- to Short-Range Order in Compositionally Disordered Soft Mode Ferroelectrics journal, July 1996

Relaxor Ferroelectrics: Back to the Single-Soft-Mode Picture journal, October 2016

Composition dependence of the diffuse scattering in the relaxor ferroelectric compound ( 1 − x ) Pb ( Mg 1 ∕ 3 Nb 2 ∕ 3 ) O 3 − x PbTiO 3 ( 0 ≤ x ≤ 0.40 ) journal, October 2006

Neutron scattering study of the relaxor ferroelectric ( 1 − x ) Pb ( Zn 1 / 3 Nb 2 / 3 ) O 3 − x PbTiO 3 journal, April 2003

Reinterpretation of the bond-valence model with bond-order formalism: An improved bond-valence-based interatomic potential for PbTiO 3 journal, September 2013

First-principles studies of the local structure and relaxor behavior of Pb ( Mg 1 / 3 Nb 2 / 3 ) O 3 − PbTiO 3 -derived ferroelectric perovskite solid solutions journal, May 2018

Molecular Dynamics Study of Dielectric Response in a Relaxor Ferroelectric journal, November 2009

Role of substrate on the dielectric and piezoelectric behavior of epitaxial lead magnesium niobate-lead titanate relaxor thin films journal, July 2000

Negative-pressure-induced enhancement in a freestanding ferroelectric journal, August 2015

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

Strain Tuning of Ferroelectric Thin Films journal, August 2007

Seeing the forest and the trees journal, April 2012

Reinterpretation of bond-valence model with bond-order formalism: an improved bond-valence based interatomic potential for PbTiO$_3$ text, January 2012

Anisotropic Local Correlations and Dynamics in a Relaxor Ferroelectric text, January 2012

Emerging Conductive Atomic Force Microscopy for Metal Halide Perovskite Materials and Solar Cells journal, March 2020

Sr-induced dipole scatter in Ba x Sr 1 − x TiO 3 : Insights from a transferable-bond valence-based interatomic potential journal, November 2019

The giant electromechanical response in ferroelectric relaxors as a critical phenomenon
journal, June 2006

Intermediate temperature scale $T^{*}$ in lead-based relaxor systems
journal, August 2009

Crystalline ferroelectrics with glassy polarization behavior
journal, September 1983

Ultrahigh piezoelectricity in ferroelectric ceramics by design
journal, March 2018

Thin-film ferroelectric materials and their applications
journal, November 2016

Tuning Susceptibility via Misfit Strain in Relaxed Morphotropic Phase Boundary PbZr _1-x Ti _x O ₃ Epitaxial Thin Films
journal, May 2014

Pressure-Induced Suppression of the Diffuse Scattering in the Model Relaxor Ferroelectric ${P b M g}_{1 / 3} {N b}_{2 / 3} O_{3}$
journal, June 2003

Electric-field-induced redistribution of polar nano-regions in a relaxor ferroelectric
journal, January 2006

Ultrahigh strain and piezoelectric behavior in relaxor based ferroelectric single crystals
journal, August 1997

Ferroelectricity and Self-Polarization in Ultrathin Relaxor Ferroelectric Films
journal, January 2016

X-ray and neutron diffraction investigations of the structural phase transformation sequence under electric field in 0.7Pb(Mg1∕3Nb2∕3)-0.3PbTiO3 crystal
journal, August 2004

The relation of local order to material properties in relaxor ferroelectrics
journal, June 2018

Properties of Epitaxial Films Made of Relaxor Ferroelectrics
journal, December 2013

Diffuse X-Ray Scattering Study of Lead Magnesium Niobate Single Crystals
journal, November 1997

Crystal Structure and Pair Potentials: A Molecular-Dynamics Study
journal, October 1980

Three-dimensional mapping of diffuse scattering in $Pb ({Zn}_{1 ∕ 3} {Nb}_{2 ∕ 3}) O_{3} − x Pb Ti O_{3}$
journal, November 2004

Relationship between Local Structure and Relaxor Behavior in Perovskite Oxides
journal, December 2007

Relaxorferroelectrics: An overview
journal, January 1994

Low-temperature relaxor state induced by epitaxial compression in PbSc $_{0.5}$ Nb $_{0.5}$ O $_{3}$ films
journal, June 2013

Visualization of dielectric constant-electric field-temperature phase maps for imprinted relaxor ferroelectric thin films
journal, March 2016

Diffuse scattering in relaxor ferroelectrics: true three-dimensional mapping, experimental artefacts and modelling
journal, November 2011

Anisotropic Local Correlations and Dynamics in a Relaxor Ferroelectric
journal, April 2013

Do we need the Ether of Polar Nanoregions?
journal, April 2012

Perovskite phase stabilization in epitaxial Pb(Mg1/3Nb2/3)O3–PbTiO3 films by deposition onto vicinal (001) SrTiO3 substrates
journal, November 2001

In-situ neutron diffraction study of Pb(In _1/2 Nb _1/2 )O ₃ -Pb(Mg _1/3 Nb _2/3 )O ₃ -PbTiO ₃ single crystals under uniaxial mechanical stress
journal, April 2012

Observation of Nanoscale $180 °$ Stripe Domains in Ferroelectric ${P b T i O}_{3}$ Thin Films
journal, July 2002

Effect of Mechanical Boundary Conditions on Phase Diagrams of Epitaxial Ferroelectric Thin Films
journal, March 1998

Uniaxial-stress induced phase transitions in [001]C-poled 0.955Pb(Zn1∕3Nb2∕3)O3–0.045PbTiO3
journal, April 2007

Self-Accommodation of Ionic Size-Effect Atomic Displacements in Antiferroelectric Order in Relaxor Lead Scandium Niobate
journal, May 1999

Phase instability induced by polar nanoregions in a relaxor ferroelectric system
journal, May 2008

Relationship between local structure and phase transitions of a disordered solid solution
journal, October 2002

Effect of mechanical constraint on the dielectric and piezoelectric behavior of epitaxial Pb(Mg1/3Nb2/3)O3(90%)–PbTiO3(10%) relaxor thin films
journal, December 1999

Seeing the forest and the trees
journal, June 2018

Neutron elastic diffuse scattering study of $Pb ({Mg}_{1 / 3} {Nb}_{2 / 3}) O_{3}$
journal, February 2004

Epitaxial Ferroelectric Heterostructures Fabricated by Selective Area Epitaxy of SrRuO3 Using an MgO Mask
journal, February 2012

Pressure-Induced Crossover from Long- to Short-Range Order in Compositionally Disordered Soft Mode Ferroelectrics
journal, July 1996

Relaxor Ferroelectrics: Back to the Single-Soft-Mode Picture
journal, October 2016

Composition dependence of the diffuse scattering in the relaxor ferroelectric compound $(1 - x) Pb ({Mg}_{1 ∕ 3} {Nb}_{2 ∕ 3}) O_{3} - x {PbTiO}_{3} (0 \leq x \leq 0.40)$
journal, October 2006

Neutron scattering study of the relaxor ferroelectric $(1 - x) Pb ({Zn}_{1 / 3} {Nb}_{2 / 3}) O_{3} - x {PbTiO}_{3}$
journal, April 2003

Reinterpretation of the bond-valence model with bond-order formalism: An improved bond-valence-based interatomic potential for PbTiO $_{3}$
journal, September 2013

First-principles studies of the local structure and relaxor behavior of ${Pb (Mg}_{1 / 3} {Nb}_{2 / 3}) O_{3} − {PbTiO}_{3}$ -derived ferroelectric perovskite solid solutions
journal, May 2018

Molecular Dynamics Study of Dielectric Response in a Relaxor Ferroelectric
journal, November 2009

Role of substrate on the dielectric and piezoelectric behavior of epitaxial lead magnesium niobate-lead titanate relaxor thin films
journal, July 2000

Negative-pressure-induced enhancement in a freestanding ferroelectric
journal, August 2015

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

Strain Tuning of Ferroelectric Thin Films
journal, August 2007

Seeing the forest and the trees
journal, April 2012

Reinterpretation of bond-valence model with bond-order formalism: an improved bond-valence based interatomic potential for PbTiO$_3$
text, January 2012

Anisotropic Local Correlations and Dynamics in a Relaxor Ferroelectric
text, January 2012

Emerging Conductive Atomic Force Microscopy for Metal Halide Perovskite Materials and Solar Cells
journal, March 2020

Sr-induced dipole scatter in ${Ba}_{x} {Sr}_{1 - x} {TiO}_{3}$ : Insights from a transferable-bond valence-based interatomic potential
journal, November 2019