Stabilization of Polar Nanoregions in Pb-free Ferroelectrics

Pramanick, A.; Dmowski, Wojciech; Egami, Takeshi; Budisuharto, A. Setiadi; Weyland, F.; Novak, N.; Christianson, Andrew D.; Borreguero, J. M.; Abernathy, Douglas L.; Jorgensen, M. R. V.

doi:10.1103/PhysRevLett.120.207603

Title: Stabilization of Polar Nanoregions in Pb-free Ferroelectrics

Abstract

In this study, the formation of polar nanoregions through solid-solution additions is known to enhance significantly the functional properties of ferroelectric materials. Despite considerable progress in characterizing the microscopic behavior of polar nanoregions (PNR), understanding their real-space atomic structure and dynamics of their formation remains a considerable challenge. Here, using the method of dynamic pair distribution function, we provide direct insights into the role of solid-solution additions towards the stabilization of polar nanoregions in the Pb-free ferroelectric of Ba(Zr,Ti)O₃. It is shown that for an optimum level of substitution of Ti by larger Zr ions, the dynamics of atomic displacements for ferroelectric polarization are slowed sufficiently below THz frequencies, which leads to increased local correlation among dipoles within PNRs. The dynamic pair distribution function technique demonstrates a unique capability to obtain insights into locally correlated atomic dynamics in disordered materials, including new Pb-free ferroelectrics, which is necessary to understand and control their functional properties.

Authors:

Pramanick, A. ^[1]; Dmowski, Wojciech ^[2]; Egami, Takeshi ^[2]; Budisuharto, A. Setiadi ^[1]; Weyland, F. ^[3]; Novak, N. ^[3];

^[4];

^[4]; Jorgensen, M. R. V. ^[5]

City Univ. of Hong Kong, Kowloon Tong (Hong Kong SAR)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Oak Ridge, TN (United States)
Technische Univ. Darmstadt, Darmstadt (Germany)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Aarhus Univ., Aarhus C (Denmark); Lund Univ., Lund (Sweden)

Publication Date:: Fri May 18 00:00:00 EDT 2018

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

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

OSTI Identifier:: 1440833

Alternate Identifier(s):: OSTI ID: 1437680

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Letters

Additional Journal Information:: Journal Volume: 120; Journal Issue: 20; Journal ID: ISSN 0031-9007

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Pramanick, A., Dmowski, Wojciech, Egami, Takeshi, Budisuharto, A. Setiadi, Weyland, F., Novak, N., Christianson, Andrew D., Borreguero, J. M., Abernathy, Douglas L., and Jorgensen, M. R. V. Stabilization of Polar Nanoregions in Pb-free Ferroelectrics.  United States: N. p., 2018. 
Web.  doi:10.1103/PhysRevLett.120.207603.

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                    Pramanick, A., Dmowski, Wojciech, Egami, Takeshi, Budisuharto, A. Setiadi, Weyland, F., Novak, N., Christianson, Andrew D., Borreguero, J. M., Abernathy, Douglas L., & Jorgensen, M. R. V. Stabilization of Polar Nanoregions in Pb-free Ferroelectrics.  United States.  https://doi.org/10.1103/PhysRevLett.120.207603

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                    Pramanick, A., Dmowski, Wojciech, Egami, Takeshi, Budisuharto, A. Setiadi, Weyland, F., Novak, N., Christianson, Andrew D., Borreguero, J. M., Abernathy, Douglas L., and Jorgensen, M. R. V. Fri .  
"Stabilization of Polar Nanoregions in Pb-free Ferroelectrics".  United States.  https://doi.org/10.1103/PhysRevLett.120.207603.  https://www.osti.gov/servlets/purl/1440833.

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@article{osti_1440833,

  title        = {Stabilization of Polar Nanoregions in Pb-free Ferroelectrics},

  author       = {Pramanick, A. and Dmowski, Wojciech and Egami, Takeshi and Budisuharto, A. Setiadi and Weyland, F. and Novak, N. and Christianson, Andrew D. and Borreguero, J. M. and Abernathy, Douglas L. and Jorgensen, M. R. V.},

  abstractNote = {In this study, the formation of polar nanoregions through solid-solution additions is known to enhance significantly the functional properties of ferroelectric materials. Despite considerable progress in characterizing the microscopic behavior of polar nanoregions (PNR), understanding their real-space atomic structure and dynamics of their formation remains a considerable challenge. Here, using the method of dynamic pair distribution function, we provide direct insights into the role of solid-solution additions towards the stabilization of polar nanoregions in the Pb-free ferroelectric of Ba(Zr,Ti)O3. It is shown that for an optimum level of substitution of Ti by larger Zr ions, the dynamics of atomic displacements for ferroelectric polarization are slowed sufficiently below THz frequencies, which leads to increased local correlation among dipoles within PNRs. The dynamic pair distribution function technique demonstrates a unique capability to obtain insights into locally correlated atomic dynamics in disordered materials, including new Pb-free ferroelectrics, which is necessary to understand and control their functional properties.},

  doi          = {10.1103/PhysRevLett.120.207603},

  journal      = {Physical Review Letters},

  number       = 20,

  volume       = 120,

  place        = {United States},

  year         = {Fri May 18 00:00:00 EDT 2018},

  month        = {Fri May 18 00:00:00 EDT 2018}

}

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https://doi.org/10.1103/PhysRevLett.120.207603

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Cited by: 41 works

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Figures / Tables:

Figure 1: (a) Phase diagram of Ba(Zr_xTi_1-x)O₃. The compositions used for the current study are shown by dotted lines. (b) Dielectric permittivity $ε_{r}$ as a function of temperature for different x. (c) Comparison of P-E hysteresis loops for x = 0.10 and x = 0.15. The decrease in coercive 11more »

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Title: Stabilization of Polar Nanoregions in Pb-free Ferroelectrics

Abstract

Citation Formats

Figures / Tables:

Anisotropy of the Electrocaloric Effect in Lead-Free Relaxor Ferroelectrics journal, March 2014

Polymorphic phase boundaries and enhanced piezoelectric response in extended composition range in the lead free ferroelectric BaTi 1−x Zr x O 3 journal, July 2013

One hundred years of diffuse scattering journal, July 2015

Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments journal, November 2014

Average and local atomic-scale structure in BaZr x Ti 1− x O 3 ( x = 0.10, 0.20, 0.40) ceramics by high-energy x-ray diffraction and Raman spectroscopy journal, January 2014

Broad-band dielectric response of PbMg1/3Nb2/3O3 relaxor ferroelectrics: Single crystals, ceramics and thin films journal, January 2006

Giant electromechanical coupling of relaxor ferroelectrics controlled by polar nanoregion vibrations journal, September 2016

Dynamic pair-density function method for neutron and X-ray inelastic scattering journal, May 2012

Coexistence of the Phonon and Relaxation Soft Modes in the Terahertz Dielectric Response of Tetragonal BaTiO 3 journal, October 2008

Large Piezoelectric Effect in Pb-Free Ceramics journal, December 2009

Evidence for charge localization in the ferromagnetic phase of La 1 − x Ca x MnO 3 from high real-space-resolution x-ray diffraction journal, July 2000

Phonon localization drives polar nanoregions in a relaxor ferroelectric journal, April 2014

Finite-Temperature Properties of Ba ( Zr , Ti ) O 3 Relaxors from First Principles journal, June 2012

Observation of dynamic atom-atom correlation in liquid helium in real space journal, May 2017

Microdomain dynamics in single-crystal BaTi O 3 during paraelectric-ferroelectric phase transition measured with time-of-flight neutron scattering journal, November 2015

Correspondence: Reply to ‘Phantom phonon localization in relaxors’ journal, December 2017

Origin of ferroelectricity in perovskite oxides journal, July 1992

Neutron-Scattering Study of Soft Modes in Cubic BaTi O 3 journal, July 1971

Electrocaloric materials for future solid-state refrigeration technologies journal, July 2012

Giant Electrocaloric Response Over A Broad Temperature Range in Modified BaTiO 3 Ceramics journal, September 2013

Subterahertz dielectric relaxation in lead-free Ba(Zr,Ti)O3 relaxor ferroelectrics journal, April 2016

A comparison of various commonly used correlation functions for describing total scattering journal, April 2001

Two-dimensional mapping of polarizations of rhombohedral nanostructures in the tetragonal phase of BaTiO 3 by the combined use of the scanning transmission electron microscopy and convergent-beam electron diffraction methods journal, August 2013

Coupling and competition between ferroelectricity, magnetism, strain, and oxygen vacancies in A MnO 3 perovskites journal, August 2016

Local Lattice Dynamics and the Origin of the Relaxor Ferroelectric Behavior journal, April 2008

Lead-free piezoceramics journal, October 2004

Colloquium : Theory of intertwined orders in high temperature superconductors journal, May 2015

Complexity in Strongly Correlated Electronic Systems journal, July 2005

The chain structure of BaTiO3 and KNbO3 journal, October 1968

Anomalous Phase Diagram of Ferroelectric ( Ba , Ca ) TiO 3 Single Crystals with Giant Electromechanical Response journal, June 2008

Skyrmion Lattice in a Chiral Magnet journal, February 2009

Perspective on the Development of Lead-free Piezoceramics journal, June 2009

Lattice dynamics and origin of ferroelectricity in BaTiO 3 : Linearized-augmented-plane-wave total-energy calculations journal, October 1990

Local structure in BaTi 1 − x Zr x O 3 relaxors from neutron pair distribution function analysis journal, February 2009

Transferring lead-free piezoelectric ceramics into application journal, June 2015

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

The Dielectric Relaxation in Solid Solutions BaTi 1-x Zr x O 3 journal, May 2009

Residual ferroelectricity in barium strontium titanate thin film tunable dielectrics journal, July 2014

Nanoscale Atomic Displacements Ordering for Enhanced Piezoelectric Properties in Lead-Free ABO 3 Ferroelectrics journal, June 2015

RMCProfile: reverse Monte Carlo for polycrystalline materials journal, July 2007

Correspondence: Phantom phonon localization in relaxors journal, December 2017

Phase Diagram of BaTi O 3 journal, March 1997

Diffuse scattering resulting from macromolecular frustration journal, October 2011

Piezoelectric response and free-energy instability in the perovskite crystals Ba Ti O 3 , Pb Ti O 3 , and Pb ( Zr , Ti ) O 3 journal, May 2006

Potassium–Sodium Niobate Lead-Free Piezoelectric Materials: Past, Present, and Future of Phase Boundaries journal, March 2015

Structurally frustrated polar nanoregions in BaTiO3-based relaxor ferroelectric systems journal, October 2007

The crystallography of correlated disorder journal, May 2015

Direct Observation of the Formation of Polar Nanoregions in Pb ( Mg 1 / 3 Nb 2 / 3 ) O 3 Using Neutron Pair Distribution Function Analysis journal, April 2005

Relaxing with relaxors: a review of relaxor ferroelectrics journal, April 2011

Origins of large enhancement in electromechanical coupling for nonpolar directions in ferroelectric BaTiO 3 journal, November 2013

Diffuse scattering and partial disorder in complex structures journal, October 2014

Shape Memory Effect and Superelasticity in a Strain Glass Alloy journal, December 2006

Compositional phase diagram and microscopic mechanism of Ba 1−x Ca x Zr y Ti 1−y O 3 relaxor ferroelectrics journal, January 2017

Broad-temperature-span and large electrocaloric effect in lead-free ceramics utilizing successive and metastable phase transitions journal, January 2019

A simple correction for the parallax effect in X-ray pair distribution function measurements journal, September 2019

Ferroelectric characteristics of Fe/Nb co-doped BaTiO 3 journal, August 2019

Real-Space Description of Dynamics of Liquids journal, October 2018

A simple correction for the parallax effect in X-ray pair distribution function measurements text, January 2019

Anisotropy of the Electrocaloric Effect in Lead-Free Relaxor Ferroelectrics
journal, March 2014

Polymorphic phase boundaries and enhanced piezoelectric response in extended composition range in the lead free ferroelectric BaTi _1−x Zr _x O ₃
journal, July 2013

One hundred years of diffuse scattering
journal, July 2015

Mantid—Data analysis and visualization package for neutron scattering and $μ$ SR experiments
journal, November 2014

Average and local atomic-scale structure in BaZr _x Ti _{1− x} O ₃ ( x = 0.10, 0.20, 0.40) ceramics by high-energy x-ray diffraction and Raman spectroscopy
journal, January 2014

Broad-band dielectric response of PbMg1/3Nb2/3O3 relaxor ferroelectrics: Single crystals, ceramics and thin films
journal, January 2006

Giant electromechanical coupling of relaxor ferroelectrics controlled by polar nanoregion vibrations
journal, September 2016

Dynamic pair-density function method for neutron and X-ray inelastic scattering
journal, May 2012

Coexistence of the Phonon and Relaxation Soft Modes in the Terahertz Dielectric Response of Tetragonal ${BaTiO}_{3}$
journal, October 2008

Large Piezoelectric Effect in Pb-Free Ceramics
journal, December 2009

Evidence for charge localization in the ferromagnetic phase of ${La}_{1 - x} {Ca}_{x} {MnO}_{3}$ from high real-space-resolution x-ray diffraction
journal, July 2000

Phonon localization drives polar nanoregions in a relaxor ferroelectric
journal, April 2014

Finite-Temperature Properties of $Ba (Zr, Ti) O_{3}$ Relaxors from First Principles
journal, June 2012

Observation of dynamic atom-atom correlation in liquid helium in real space
journal, May 2017

Microdomain dynamics in single-crystal $BaTi O_{3}$ during paraelectric-ferroelectric phase transition measured with time-of-flight neutron scattering
journal, November 2015

Correspondence: Reply to ‘Phantom phonon localization in relaxors’
journal, December 2017

Origin of ferroelectricity in perovskite oxides
journal, July 1992

Neutron-Scattering Study of Soft Modes in Cubic BaTi $O_{3}$
journal, July 1971

Electrocaloric materials for future solid-state refrigeration technologies
journal, July 2012

Giant Electrocaloric Response Over A Broad Temperature Range in Modified BaTiO ₃ Ceramics
journal, September 2013

Subterahertz dielectric relaxation in lead-free Ba(Zr,Ti)O3 relaxor ferroelectrics
journal, April 2016

A comparison of various commonly used correlation functions for describing total scattering
journal, April 2001

Two-dimensional mapping of polarizations of rhombohedral nanostructures in the tetragonal phase of BaTiO ₃ by the combined use of the scanning transmission electron microscopy and convergent-beam electron diffraction methods
journal, August 2013

Coupling and competition between ferroelectricity, magnetism, strain, and oxygen vacancies in A MnO ₃ perovskites
journal, August 2016

Local Lattice Dynamics and the Origin of the Relaxor Ferroelectric Behavior
journal, April 2008

Lead-free piezoceramics
journal, October 2004

Colloquium : Theory of intertwined orders in high temperature superconductors
journal, May 2015

Complexity in Strongly Correlated Electronic Systems
journal, July 2005

The chain structure of BaTiO3 and KNbO3
journal, October 1968

Anomalous Phase Diagram of Ferroelectric $(Ba, Ca) {TiO}_{3}$ Single Crystals with Giant Electromechanical Response
journal, June 2008

Skyrmion Lattice in a Chiral Magnet
journal, February 2009

Perspective on the Development of Lead-free Piezoceramics
journal, June 2009

Lattice dynamics and origin of ferroelectricity in ${BaTiO}_{3}$ : Linearized-augmented-plane-wave total-energy calculations
journal, October 1990

Local structure in ${BaTi}_{1 - x} {Zr}_{x} O_{3}$ relaxors from neutron pair distribution function analysis
journal, February 2009

Transferring lead-free piezoelectric ceramics into application
journal, June 2015

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

The Dielectric Relaxation in Solid Solutions BaTi _1-x Zr _x O ₃
journal, May 2009

Residual ferroelectricity in barium strontium titanate thin film tunable dielectrics
journal, July 2014

Nanoscale Atomic Displacements Ordering for Enhanced Piezoelectric Properties in Lead-Free ABO ₃ Ferroelectrics
journal, June 2015

RMCProfile: reverse Monte Carlo for polycrystalline materials
journal, July 2007

Correspondence: Phantom phonon localization in relaxors
journal, December 2017

Phase Diagram of BaTi $O_{3}$
journal, March 1997

Diffuse scattering resulting from macromolecular frustration
journal, October 2011

Piezoelectric response and free-energy instability in the perovskite crystals $Ba Ti O_{3}$ , $Pb Ti O_{3}$ , and $Pb (Zr, Ti) O_{3}$
journal, May 2006

Potassium–Sodium Niobate Lead-Free Piezoelectric Materials: Past, Present, and Future of Phase Boundaries
journal, March 2015

Structurally frustrated polar nanoregions in BaTiO3-based relaxor ferroelectric systems
journal, October 2007

The crystallography of correlated disorder
journal, May 2015

Direct Observation of the Formation of Polar Nanoregions in $Pb ({Mg}_{1 / 3} {Nb}_{2 / 3}) O_{3}$ Using Neutron Pair Distribution Function Analysis
journal, April 2005

Relaxing with relaxors: a review of relaxor ferroelectrics
journal, April 2011

Origins of large enhancement in electromechanical coupling for nonpolar directions in ferroelectric BaTiO $_{3}$
journal, November 2013

Diffuse scattering and partial disorder in complex structures
journal, October 2014

Shape Memory Effect and Superelasticity in a Strain Glass Alloy
journal, December 2006

Compositional phase diagram and microscopic mechanism of Ba _1−x Ca _x Zr _y Ti _1−y O ₃ relaxor ferroelectrics
journal, January 2017

Broad-temperature-span and large electrocaloric effect in lead-free ceramics utilizing successive and metastable phase transitions
journal, January 2019

A simple correction for the parallax effect in X-ray pair distribution function measurements
journal, September 2019

Ferroelectric characteristics of Fe/Nb co-doped BaTiO ₃
journal, August 2019

Real-Space Description of Dynamics of Liquids
journal, October 2018

A simple correction for the parallax effect in X-ray pair distribution function measurements
text, January 2019