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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

Here, we report a comprehensive structure-property phase diagram of unique single-ion type-1 multiferroic pseudocubic Sr 1-xBa xMnO 3 perovskites. Employing a specially designed multi-step reduction-oxidation synthesis technique, we describe the successful synthesis of previously unknown Sr 1-xBa xMnO 3 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 xMnO 3 is of great importance as it opens the door wide to the development of newer materials from the parent (AA’)(BB’) O 3 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/cm 2 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 tomore » 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 T N. The refined magnetic moments confirm the strong covalent bonding between Mn and the oxygen anions which is necessary for stabilizing the ferroelectric phase.« less

Authors:
 [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
Publication Date:
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:
Journal Article: 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.
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. doi:10.1103/PhysRevMaterials.2.054408.
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. doi:10.1103/PhysRevMaterials.2.054408. https://www.osti.gov/servlets/purl/1439880.
@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},
issn = {2475-9953},
number = 5,
volume = 2,
place = {United States},
year = {2018},
month = {5}
}

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