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Strain-induced tetragonal distortions and multiferroic properties in polycrystalline Sr1-x BaxMnO3 ( x=0.43-0.45 ) perovskites

Journal Article · · Physical Review Materials
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  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
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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 Lab. (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, Journal Name: Physical Review Materials Journal Issue: 5 Vol. 2; ISSN PRMHAR; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (3)

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

Figures / Tables (16)

FIG. 1(p. 14)figure FIG. 1
FIG. 2(p. 15)figure FIG. 2
FIG. 3(p. 16)figure FIG. 3
FIG. 4(p. 17)figure FIG. 4
FIG. 5(p. 18)figure FIG. 5
FIG. 6(p. 19)figure FIG. 6
FIG. 7(p. 20)figure FIG. 7
FIG. 8(p. 21)figure FIG. 8
FIG. 9(p. 22)figure FIG. 9
FIG. 10(p. 23)figure FIG. 10
FIG. 11(p. 24)figure FIG. 11
FIG. 12(p. 25)figure FIG. 12
FIG. 13(p. 26)figure FIG. 13
FIG. 14(p. 27)figure FIG. 14
FIG. 15(p. 28)figure FIG. 15
FIG. 16(p. 29)figure FIG. 16

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Related Subjects

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