Strain-induced tetragonal distortions and multiferroic properties in polycrystalline Sr1-xBaxMnO3 ( x=0.43-0.45 ) perovskites

Somaily, H.; Kolesnik, S.; Mais, J.; Brown, D.; Chapagain, K.; Dabrowski, B.; Chmaissem, O.

doi:10.1103/PhysRevMaterials.2.054408

Title: Strain-induced tetragonal distortions and multiferroic properties in polycrystalline ${Sr}_{1 - x} B a_{x} Mn O_{3}$ ( $x = 0.43 - 0.45$ ) perovskites

Abstract

Here, we report a comprehensive structure-property phase diagram of unique single-ion type-1 multiferroic pseudocubic Sr_1-xBa_xMnO₃ perovskites. Employing a specially designed multi-step reduction-oxidation synthesis technique, we describe the successful synthesis of previously unknown Sr_1-xBa_xMnO₃ compositions in their polycrystalline form with a significantly extended Ba solubility limit that is only rivaled by a very limited number of crystals and thin films grown under non-equilibrium conditions. Understanding the multiferroic interplay with structure in Sr_1-xBa_xMnO₃ is of great importance as it opens the door wide to the development of newer materials from the parent (AA’)(BB’) O₃ system with enhanced properties. To this end, using a combination of time-of-flight neutron and synchrotron x-ray scattering techniques, we determined the exact structures and quantified the Mn and oxygen polar distortions above and below T_C and T_N. In its ferroelectric state, the system crystalizes in the noncentrosymmetric tetragonal P4mm space group which gives rise to a large electric dipole moment P_s, in the z-direction, of 18.4 and 29.5 µC/cm² for x = 0.43 and 0.45, respectively. The two independently driven ferroelectric and magnetic order parameters are single-handedly accommodated by the Mn sublattice leading to a novel strain-assisted multiferroic behavior in agreement with many theoretical predictions. Our neutron diffractionmore »« less

Authors:

Somaily, H. ^[1]; Kolesnik, S. ^[1]; Mais, J. ^[1]; Brown, D. ^[1]; Chapagain, K. ^[1]; Dabrowski, B. ^[1]; Chmaissem, O. ^[2]

Northern Illinois Univ., DeKalb, IL (United States). Dept. of Physics
Northern Illinois Univ., DeKalb, IL (United States). Dept. of Physics; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

Publication Date:: 2018-05-17

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

OSTI Identifier:: 1439880

Alternate Identifier(s):: OSTI ID: 1437518

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Materials

Additional Journal Information:: Journal Volume: 2; Journal Issue: 5; Journal ID: ISSN 2475-9953

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; antiferromagnetism; ferroelectricity; magnetism; structural properties; neutron diffraction

Citation Formats


                    Somaily, H., Kolesnik, S., Mais, J., Brown, D., Chapagain, K., Dabrowski, B., and Chmaissem, O. Strain-induced tetragonal distortions and multiferroic properties in polycrystalline Sr1-xBaxMnO3 ( x=0.43-0.45 ) perovskites.  United States: N. p., 2018. 
Web.  doi:10.1103/PhysRevMaterials.2.054408.

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                    Somaily, H., Kolesnik, S., Mais, J., Brown, D., Chapagain, K., Dabrowski, B., & Chmaissem, O. Strain-induced tetragonal distortions and multiferroic properties in polycrystalline Sr1-xBaxMnO3 ( x=0.43-0.45 ) perovskites.  United States.  https://doi.org/10.1103/PhysRevMaterials.2.054408

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                    Somaily, H., Kolesnik, S., Mais, J., Brown, D., Chapagain, K., Dabrowski, B., and Chmaissem, O. Thu .  
"Strain-induced tetragonal distortions and multiferroic properties in polycrystalline Sr1-xBaxMnO3 ( x=0.43-0.45 ) perovskites".  United States.  https://doi.org/10.1103/PhysRevMaterials.2.054408.  https://www.osti.gov/servlets/purl/1439880.

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@article{osti_1439880,

  title        = {Strain-induced tetragonal distortions and multiferroic properties in polycrystalline Sr1-xBaxMnO3 ( x=0.43-0.45 ) perovskites},

  author       = {Somaily, H. and Kolesnik, S. and Mais, J. and Brown, D. and Chapagain, K. and Dabrowski, B. and Chmaissem, O.},

  abstractNote = {Here, we report a comprehensive structure-property phase diagram of unique single-ion type-1 multiferroic pseudocubic Sr1-xBaxMnO3 perovskites. Employing a specially designed multi-step reduction-oxidation synthesis technique, we describe the successful synthesis of previously unknown Sr1-xBaxMnO3 compositions in their polycrystalline form with a significantly extended Ba solubility limit that is only rivaled by a very limited number of crystals and thin films grown under non-equilibrium conditions. Understanding the multiferroic interplay with structure in Sr1-xBaxMnO3 is of great importance as it opens the door wide to the development of newer materials from the parent (AA’)(BB’) O3 system with enhanced properties. To this end, using a combination of time-of-flight neutron and synchrotron x-ray scattering techniques, we determined the exact structures and quantified the Mn and oxygen polar distortions above and below TC and TN. In its ferroelectric state, the system crystalizes in the noncentrosymmetric tetragonal P4mm space group which gives rise to a large electric dipole moment Ps, in the z-direction, of 18.4 and 29.5 µC/cm2 for x = 0.43 and 0.45, respectively. The two independently driven ferroelectric and magnetic order parameters are single-handedly accommodated by the Mn sublattice leading to a novel strain-assisted multiferroic behavior in agreement with many theoretical predictions. Our neutron diffraction results demonstrate the large and tunable suppression of the ferroelectric order at the onset of AFM ordering and confirm the coexistence and strong coupling of the two ferroic orders below TN. The refined magnetic moments confirm the strong covalent bonding between Mn and the oxygen anions which is necessary for stabilizing the ferroelectric phase.},

  doi          = {10.1103/PhysRevMaterials.2.054408},

  journal      = {Physical Review Materials},

  number       = 5,

  volume       = 2,

  place        = {United States},

  year         = {2018},

  month        = {5}

}

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Figures / Tables:

FIG. 1: Thermogravimetric analysis measurements for the as-synthesized Sr_0.55Ba_0.45MnO_3-d sample on heating and cooling (indicated by arrows) in pure oxygen at 1 K/min and held at 670 K for four hours. Inset: Oxygen nonstoichiometry during heating and cooling the perovskite phases Sr_1-xBa_xMnO_3-d (x = 0.0, 0.1, 0.2, 0.3, 0.4) inmore »

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Works referencing / citing this record:

Engineering the magnetic order in epitaxially strained Sr _1−x Ba _x MnO ₃ perovskite thin films
journal, April 2019

Maurel, L.; Marcano, N.; Langenberg, E.
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Tunable multiferroic order parameters in $S r_{1 - x} B a_{x} M n_{1 - y} T i_{y} O_{3}$
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Chapagain, Kamal; Brown, Dennis E.; Kolesnik, Stanislaw
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Engineering the magnetic order in epitaxially strained Sr1−xBaxMnO3 perovskite thin films
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Maurel, Laura; Marcano, N.; Langenberg, Eric
ETH Zurich
DOI: 10.3929/ethz-b-000340648

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Title: Strain-induced tetragonal distortions and multiferroic properties in polycrystalline Sr 1 - x B a x Mn O 3 ( x = 0.43 - 0.45 ) perovskites

Abstract

Citation Formats

Figures / Tables:

Room-temperature ferroelectricity in strained SrTiO3 journal, August 2004

Structural parameters and electron difference density in BaTiO3 journal, December 1992

Soft phonon mode coupled with antiferromagnetic order in incipient-ferroelectric Mott insulators Sr 1 − x Ba x MnO 3 journal, September 2012

Magnetic control of ferroelectric polarization journal, November 2003

Spectroscopic studies of the ferroelectric and magnetic phase transitions in multiferroic Sr 1− x Ba x MnO 3 journal, March 2016

Epitaxial-Strain-Induced Multiferroicity in SrMnO 3 from First Principles journal, May 2010

Phase diagram of Sr 1 − x Ba x MnO 3 as a function of chemical doping, epitaxial strain, and external pressure journal, October 2016

EXPGUI , a graphical user interface for GSAS journal, April 2001

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal, September 1976

Tolerance factor rules for Sr1−x−yCaxBayMnO3 perovskites journal, January 2003

Relationship between structural parameters and the Néel temperature in Sr 1 − x Ca x MnO 3 ( 0 <~ x <~ 1 ) and Sr 1 − y Ba y MnO 3 ( y <~ 0 . 2 ) journal, September 2001

Origin of multiferroic spiral spin order in the R MnO 3 perovskites journal, October 2008

Effects of internal structural parameters on the properties of Ba-substituted La 0.5 Sr 0.5 Mn O 3 journal, October 2006

The system SrMnO3−x journal, April 1970

Displacement-Type Ferroelectricity with Off-Center Magnetic Ions in Perovskite Sr 1 − x Ba x MnO 3 journal, September 2011

Magnetically Induced Electronic Ferroelectricity in Half-Doped Manganites journal, July 2009

Multiferroic phase competitions in perovskite manganite thin films journal, January 2012

Coexistence of magnetism and ferroelectricity in perovskites journal, May 2002

Microscopic model and phase diagrams of the multiferroic perovskite manganites journal, October 2009

Non- d 0 Mn-driven ferroelectricity in antiferromagnetic BaMnO 3 journal, May 2009

Theoretical Model for Explaining the Ferroelectric Effect in Barium Titanate journal, December 1948

Electric polarization of Sr 0.5 Ba 0.5 MnO 3 : A multiferroic Mott insulator journal, December 2014

Novel Properties of Atomically Arranged Perovskites journal, January 2007

Origin of ferroelectricity in perovskite oxides journal, July 1992

Magnetic Structure of the Cubic Perovskite Type SrMnO 3 journal, July 1974

Electronic and ionic transport properties and other physical aspects of perovskites journal, September 2004

Neutron scattering studies of the ferroelectric distortion and spin dynamics in the type-1 multiferroic perovskite Sr 0.56 Ba 0.44 MnO 3 journal, October 2014

Engineering Multiferroism in CaMnO 3 journal, March 2009

Multiferroics progress and prospects in thin films journal, January 2007

Multiferroicity due to charge ordering journal, October 2008

Multiferroics: a magnetic twist for ferroelectricity journal, January 2007

Microscopic Origin of Large Negative Magnetoelectric Coupling in Sr 1 / 2 Ba 1 / 2 MnO 3 journal, September 2012

Multiferroicity: the coupling between magnetic and polarization orders journal, July 2009

Enhancement of Ferroelectricity in Strained BaTiO3 Thin Films journal, November 2004

Universal Octahedral-Site Distortion in Orthorhombic Perovskite Oxides journal, February 2005

Domain Structure and Dielectric Response of Barium Titanate Single Crystals journal, June 1948

Ferroelectric transition in Y Mn O 3 from first principles journal, September 2005

Intrinsic structural distortion in orthorhombic perovskite oxides journal, April 2008

Spin-phonon coupling in epitaxial S r 0.6 B a 0.4 Mn O 3 thin films journal, February 2017

Phase Transitions in BaTi O 3 from First Principles journal, September 1994

Controlling the Electrical and Magnetoelectric Properties of Epitaxially Strained Sr 1− x Ba x MnO 3 Thin Films journal, February 2017

Magnetoelectric phase diagrams of orthorhombic R MnO 3 ( R = Gd , Tb, and Dy) journal, June 2005

Cation disorder and size effects in magnetoresistive manganese oxide perovskites journal, December 1996

Epitaxial BiFeO3 Multiferroic Thin Film Heterostructures journal, March 2003

Magnetocapacitance effect in multiferroic BiMnO 3 journal, May 2003

Orbital Physics in Transition-Metal Oxides journal, April 2000

Electronic structure and magnetic properties of cubic and hexagonal Sr Mn O 3 journal, October 2006

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

Engineering the magnetic order in epitaxially strained Sr 1−x Ba x MnO 3 perovskite thin films journal, April 2019

Tunable multiferroic order parameters in S r 1 − x B a x M n 1 − y T i y O 3 journal, August 2019

Engineering the magnetic order in epitaxially strained Sr1−xBaxMnO3 perovskite thin films text, January 2019

Title: Strain-induced tetragonal distortions and multiferroic properties in polycrystalline ${Sr}_{1 - x} B a_{x} Mn O_{3}$ ( $x = 0.43 - 0.45$ ) perovskites

Room-temperature ferroelectricity in strained SrTiO₃
journal, August 2004

Structural parameters and electron difference density in BaTiO3
journal, December 1992

Soft phonon mode coupled with antiferromagnetic order in incipient-ferroelectric Mott insulators Sr $_{1 - x}$ Ba $_{x}$ MnO $_{3}$
journal, September 2012

Magnetic control of ferroelectric polarization
journal, November 2003

Spectroscopic studies of the ferroelectric and magnetic phase transitions in multiferroic Sr _{1− x} Ba _x MnO ₃
journal, March 2016

Epitaxial-Strain-Induced Multiferroicity in ${SrMnO}_{3}$ from First Principles
journal, May 2010

Phase diagram of ${Sr}_{1 - x} {Ba}_{x} {MnO}_{3}$ as a function of chemical doping, epitaxial strain, and external pressure
journal, October 2016

EXPGUI , a graphical user interface for GSAS
journal, April 2001

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Tolerance factor rules for Sr1−x−yCaxBayMnO3 perovskites
journal, January 2003

Relationship between structural parameters and the Néel temperature in ${Sr}_{1 - x} {Ca}_{x} {MnO}_{3}$ $(0 <~ x <~ 1)$ and ${Sr}_{1 - y} {Ba}_{y} {MnO}_{3}$ $(y <~ 0.2)$
journal, September 2001

Origin of multiferroic spiral spin order in the $R {MnO}_{3}$ perovskites
journal, October 2008

Effects of internal structural parameters on the properties of Ba-substituted ${La}_{0.5} {Sr}_{0.5} Mn O_{3}$
journal, October 2006

The system SrMnO3−x
journal, April 1970

Displacement-Type Ferroelectricity with Off-Center Magnetic Ions in Perovskite ${Sr}_{1 - x} {Ba}_{x} {MnO}_{3}$
journal, September 2011

Magnetically Induced Electronic Ferroelectricity in Half-Doped Manganites
journal, July 2009

Multiferroic phase competitions in perovskite manganite thin films
journal, January 2012

Coexistence of magnetism and ferroelectricity in perovskites
journal, May 2002

Microscopic model and phase diagrams of the multiferroic perovskite manganites
journal, October 2009

Non- $d^{0}$ Mn-driven ferroelectricity in antiferromagnetic ${BaMnO}_{3}$
journal, May 2009

Theoretical Model for Explaining the Ferroelectric Effect in Barium Titanate
journal, December 1948

Electric polarization of ${Sr}_{0.5} {Ba}_{0.5} {MnO}_{3}$ : A multiferroic Mott insulator
journal, December 2014

Novel Properties of Atomically Arranged Perovskites
journal, January 2007

Origin of ferroelectricity in perovskite oxides
journal, July 1992

Magnetic Structure of the Cubic Perovskite Type SrMnO ₃
journal, July 1974

Electronic and ionic transport properties and other physical aspects of perovskites
journal, September 2004

Neutron scattering studies of the ferroelectric distortion and spin dynamics in the type-1 multiferroic perovskite ${Sr}_{0.56} {Ba}_{0.44} {MnO}_{3}$
journal, October 2014

Engineering Multiferroism in ${CaMnO}_{3}$
journal, March 2009

Multiferroics progress and prospects in thin films
journal, January 2007

Multiferroicity due to charge ordering
journal, October 2008

Multiferroics: a magnetic twist for ferroelectricity
journal, January 2007

Microscopic Origin of Large Negative Magnetoelectric Coupling in ${Sr}_{1 / 2} {Ba}_{1 / 2} {MnO}_{3}$
journal, September 2012

Multiferroicity: the coupling between magnetic and polarization orders
journal, July 2009

Enhancement of Ferroelectricity in Strained BaTiO₃ Thin Films
journal, November 2004

Universal Octahedral-Site Distortion in Orthorhombic Perovskite Oxides
journal, February 2005

Domain Structure and Dielectric Response of Barium Titanate Single Crystals
journal, June 1948

Ferroelectric transition in $Y Mn O_{3}$ from first principles
journal, September 2005

Intrinsic structural distortion in orthorhombic perovskite oxides
journal, April 2008

Spin-phonon coupling in epitaxial $S r_{0.6} B a_{0.4} Mn O_{3}$ thin films
journal, February 2017

Phase Transitions in BaTi $O_{3}$ from First Principles
journal, September 1994

Controlling the Electrical and Magnetoelectric Properties of Epitaxially Strained Sr ₁₋ _x Ba _x MnO ₃ Thin Films
journal, February 2017

Magnetoelectric phase diagrams of orthorhombic $R {MnO}_{3}$ ( $R = Gd$ , Tb, and Dy)
journal, June 2005

Cation disorder and size effects in magnetoresistive manganese oxide perovskites
journal, December 1996

Epitaxial BiFeO₃ Multiferroic Thin Film Heterostructures
journal, March 2003

Magnetocapacitance effect in multiferroic ${BiMnO}_{3}$
journal, May 2003

Orbital Physics in Transition-Metal Oxides
journal, April 2000

Electronic structure and magnetic properties of cubic and hexagonal $Sr Mn O_{3}$
journal, October 2006

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

Engineering the magnetic order in epitaxially strained Sr _1−x Ba _x MnO ₃ perovskite thin films
journal, April 2019

Tunable multiferroic order parameters in $S r_{1 - x} B a_{x} M n_{1 - y} T i_{y} O_{3}$
journal, August 2019

Engineering the magnetic order in epitaxially strained Sr1−xBaxMnO3 perovskite thin films
text, January 2019