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Title: Dimensional control of defect dynamics in perovskite oxide superlattices

Abstract

Point defects play a critical role in the structural, physical, and interfacial properties of perovskite oxide superlattices. However, understanding of the fundamental properties of point defects in superlattices, especially their transport properties, is rather limited. Here, we report predictions of the stability and dynamics of oxygen vacancies in SrTiO 3/PbTiO 3 oxide superlattices using first-principles calculations in combination with the kinetic Monte Carlo method. By varying the stacking period, i.e., changing of n in nSTO/ nPTO, we discover a crossover from three-dimensional diffusion to primarily two-dimensional planar diffusion. Such planar diffusion may lead to novel designs of ionic conductors. We show that the dominant vacancy position may vary in the superlattices, depending on the superlattice structure and stacking period, contradicting the common assumption that point defects reside at interfaces. Moreover, we predict a significant increase in room-temperature ionic conductivity for 3STO/3PTO relative to the bulk phases. As a result, considering the variety of cations that can be accommodated in perovskite superlattices and the potential mismatch of spin, charge, and orbitals at the interfaces, this paper identifies a pathway to control defect dynamics for technological applications.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [2];  [3]
  1. The Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. The Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1464019
Alternate Identifier(s):
OSTI ID: 1424810
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 3; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Bredeson, Isaac, Zhang, Lipeng, Kent, Paul R. C., Cooper, Valentino R., and Xu, Haixuan. Dimensional control of defect dynamics in perovskite oxide superlattices. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.035401.
Bredeson, Isaac, Zhang, Lipeng, Kent, Paul R. C., Cooper, Valentino R., & Xu, Haixuan. Dimensional control of defect dynamics in perovskite oxide superlattices. United States. doi:10.1103/PhysRevMaterials.2.035401.
Bredeson, Isaac, Zhang, Lipeng, Kent, Paul R. C., Cooper, Valentino R., and Xu, Haixuan. Thu . "Dimensional control of defect dynamics in perovskite oxide superlattices". United States. doi:10.1103/PhysRevMaterials.2.035401. https://www.osti.gov/servlets/purl/1464019.
@article{osti_1464019,
title = {Dimensional control of defect dynamics in perovskite oxide superlattices},
author = {Bredeson, Isaac and Zhang, Lipeng and Kent, Paul R. C. and Cooper, Valentino R. and Xu, Haixuan},
abstractNote = {Point defects play a critical role in the structural, physical, and interfacial properties of perovskite oxide superlattices. However, understanding of the fundamental properties of point defects in superlattices, especially their transport properties, is rather limited. Here, we report predictions of the stability and dynamics of oxygen vacancies in SrTiO3/PbTiO3 oxide superlattices using first-principles calculations in combination with the kinetic Monte Carlo method. By varying the stacking period, i.e., changing of n in nSTO/nPTO, we discover a crossover from three-dimensional diffusion to primarily two-dimensional planar diffusion. Such planar diffusion may lead to novel designs of ionic conductors. We show that the dominant vacancy position may vary in the superlattices, depending on the superlattice structure and stacking period, contradicting the common assumption that point defects reside at interfaces. Moreover, we predict a significant increase in room-temperature ionic conductivity for 3STO/3PTO relative to the bulk phases. As a result, considering the variety of cations that can be accommodated in perovskite superlattices and the potential mismatch of spin, charge, and orbitals at the interfaces, this paper identifies a pathway to control defect dynamics for technological applications.},
doi = {10.1103/PhysRevMaterials.2.035401},
journal = {Physical Review Materials},
number = 3,
volume = 2,
place = {United States},
year = {2018},
month = {3}
}

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Cited by: 2 works
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Figures / Tables:

Figure 1 Figure 1: Top) Crystal structure of ferroelectric and paraelectric 4STO/4PTO oxide superlattices. a,b) The defect formation energies and migration energy barriers of each phase, respectively. c,d) Site occupancy of an oxygen vacancy in ferroelectric and paraelectric 4STO/4PTO. e,f) Time distribution representing in which layer the defect spend the most ofmore » its time. The interfacial TiO2 layers are highlighted in orange color.« less

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