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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

Journal Article · · Physical Review Materials
 [1];  [1];  [1];  [1];  [1];  [1];  [2]
  1. Northern Illinois Univ., DeKalb, IL (United States). Dept. of Physics
  2. Northern Illinois Univ., DeKalb, IL (United States). Dept. of Physics; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1439880
Alternate ID(s):
OSTI ID: 1437518
Journal Information:
Physical Review Materials, Vol. 2, Issue 5; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

References (48)

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

Cited By (2)


Figures / Tables (16)