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Title: Mapping strain modulated electronic structure perturbations in mixed phase bismuth ferrite thin films

Abstract

Strain engineering of epitaxial ferroelectrics has emerged as a powerful method to tailor the electromechanical response of these materials, although the effect of strain at the atomic scale and the interplay between lattice displacements and electronic structure changes are not yet fully understood. Here, using a combination of scanning transmission electron microscopy (STEM) and density functional theory (DFT), we systematically probe the role of epitaxial strain in mixed phase bismuth ferrite thin films. Electron energy loss O K and Fe L2,3 edge spectra acquired across the rhombohedral (R)-tetragonal (T) phase boundary reveal progressive, and systematic changes, in electronic structure going from one phase to the other. The comparison of the acquired spectra, with theoretical simulations using DFT, suggests a breakage in the structural symmetry across the boundary due to the simultaneous presence of increasing epitaxial strain and off- axial symmetry in the T phase. This implies that the imposed epitaxial strain plays a significant role in not only changing the crystal-field geometry, but also the bonding environment surrounding the central iron cation at the interface thus providing new insights and a possible link to understand how the imposed strain could perturb magnetic ordering in the T phase BFO.

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Materials at Irradiation and Mechanical Extremes (CMIME); Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1188885
Report Number(s):
PNNL-SA-106441
48583
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Materials Chemistry C, 3(8):1835-1845
Additional Journal Information:
Journal Name: Journal of Materials Chemistry C, 3(8):1835-1845
Country of Publication:
United States
Language:
English
Subject:
Thin films; N11663; Environmental Molecular Sciences Laboratory

Citation Formats

Krishnan, P.S. Sanakara R., Aguiar, Jeffery A., Ramasse, Q. M., Kepaptsoglou, D. M., Liang, W. I., Chu, Y. H., Browning, Nigel D., Munroe, Paul R., and Nagarajan, Valanoor. Mapping strain modulated electronic structure perturbations in mixed phase bismuth ferrite thin films. United States: N. p., 2015. Web. doi:10.1039/C4TC02064B.
Krishnan, P.S. Sanakara R., Aguiar, Jeffery A., Ramasse, Q. M., Kepaptsoglou, D. M., Liang, W. I., Chu, Y. H., Browning, Nigel D., Munroe, Paul R., & Nagarajan, Valanoor. Mapping strain modulated electronic structure perturbations in mixed phase bismuth ferrite thin films. United States. doi:10.1039/C4TC02064B.
Krishnan, P.S. Sanakara R., Aguiar, Jeffery A., Ramasse, Q. M., Kepaptsoglou, D. M., Liang, W. I., Chu, Y. H., Browning, Nigel D., Munroe, Paul R., and Nagarajan, Valanoor. Thu . "Mapping strain modulated electronic structure perturbations in mixed phase bismuth ferrite thin films". United States. doi:10.1039/C4TC02064B.
@article{osti_1188885,
title = {Mapping strain modulated electronic structure perturbations in mixed phase bismuth ferrite thin films},
author = {Krishnan, P.S. Sanakara R. and Aguiar, Jeffery A. and Ramasse, Q. M. and Kepaptsoglou, D. M. and Liang, W. I. and Chu, Y. H. and Browning, Nigel D. and Munroe, Paul R. and Nagarajan, Valanoor},
abstractNote = {Strain engineering of epitaxial ferroelectrics has emerged as a powerful method to tailor the electromechanical response of these materials, although the effect of strain at the atomic scale and the interplay between lattice displacements and electronic structure changes are not yet fully understood. Here, using a combination of scanning transmission electron microscopy (STEM) and density functional theory (DFT), we systematically probe the role of epitaxial strain in mixed phase bismuth ferrite thin films. Electron energy loss O K and Fe L2,3 edge spectra acquired across the rhombohedral (R)-tetragonal (T) phase boundary reveal progressive, and systematic changes, in electronic structure going from one phase to the other. The comparison of the acquired spectra, with theoretical simulations using DFT, suggests a breakage in the structural symmetry across the boundary due to the simultaneous presence of increasing epitaxial strain and off- axial symmetry in the T phase. This implies that the imposed epitaxial strain plays a significant role in not only changing the crystal-field geometry, but also the bonding environment surrounding the central iron cation at the interface thus providing new insights and a possible link to understand how the imposed strain could perturb magnetic ordering in the T phase BFO.},
doi = {10.1039/C4TC02064B},
journal = {Journal of Materials Chemistry C, 3(8):1835-1845},
number = ,
volume = ,
place = {United States},
year = {2015},
month = {1}
}

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