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Title: On the mobility of carriers at semi-coherent oxide heterointerfaces

Abstract

In the quest to develop new materials with enhanced ionic conductivity for battery and fuel cell applications, nano-structured oxides have attracted attention. Experimental reports indicate that oxide heterointerfaces can lead to enhanced ionic conductivity, but these same reports cannot elucidate the origin of this enhancement, often vaguely referring to pipe diffusion at misfit dislocations as a potential explanation. However, this highlights the need to understand the role of misfit dislocation structure at semi-coherent oxide heterointerfaces in modifying carrier mobilities. Here, we use atomistic and kinetic Monte Carlo (KMC) simulations to develop a model of oxygen vacancy migration at SrTiO 3/MgO interfaces, chosen because the misfit dislocation structure can be modified by changing the termination chemistry. We use atomistic simulations to determine the energetics of oxygen vacancies at both SrO and TiO 2 terminated interfaces, which are then used as the basis of the KMC simulations. While this model is approximate (as revealed by select nudged elastic band calculations), it highlights the role of the misfit dislocation structure in modifying the oxygen vacancy dynamics. We find that oxygen vacancy mobility is significantly reduced at either interface, with slight differences at each interface due to the differing misfit dislocation structure. Here, wemore » conclude that if such semi-coherent oxide heterointerfaces induce enhanced ionic conductivity, it is not a consequence of higher carrier mobility.« less

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1440497
Report Number(s):
LA-UR-18-21281
Journal ID: ISSN 1463-9076; PPCPFQ
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 19; Journal Issue: 34; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dholabhai, Pratik P., Martinez, Enrique Saez, Brown, Nicholas Taylor, and Uberuaga, Blas Pedro. On the mobility of carriers at semi-coherent oxide heterointerfaces. United States: N. p., 2017. Web. doi:10.1039/C7CP04884J.
Dholabhai, Pratik P., Martinez, Enrique Saez, Brown, Nicholas Taylor, & Uberuaga, Blas Pedro. On the mobility of carriers at semi-coherent oxide heterointerfaces. United States. doi:10.1039/C7CP04884J.
Dholabhai, Pratik P., Martinez, Enrique Saez, Brown, Nicholas Taylor, and Uberuaga, Blas Pedro. Thu . "On the mobility of carriers at semi-coherent oxide heterointerfaces". United States. doi:10.1039/C7CP04884J. https://www.osti.gov/servlets/purl/1440497.
@article{osti_1440497,
title = {On the mobility of carriers at semi-coherent oxide heterointerfaces},
author = {Dholabhai, Pratik P. and Martinez, Enrique Saez and Brown, Nicholas Taylor and Uberuaga, Blas Pedro},
abstractNote = {In the quest to develop new materials with enhanced ionic conductivity for battery and fuel cell applications, nano-structured oxides have attracted attention. Experimental reports indicate that oxide heterointerfaces can lead to enhanced ionic conductivity, but these same reports cannot elucidate the origin of this enhancement, often vaguely referring to pipe diffusion at misfit dislocations as a potential explanation. However, this highlights the need to understand the role of misfit dislocation structure at semi-coherent oxide heterointerfaces in modifying carrier mobilities. Here, we use atomistic and kinetic Monte Carlo (KMC) simulations to develop a model of oxygen vacancy migration at SrTiO3/MgO interfaces, chosen because the misfit dislocation structure can be modified by changing the termination chemistry. We use atomistic simulations to determine the energetics of oxygen vacancies at both SrO and TiO2 terminated interfaces, which are then used as the basis of the KMC simulations. While this model is approximate (as revealed by select nudged elastic band calculations), it highlights the role of the misfit dislocation structure in modifying the oxygen vacancy dynamics. We find that oxygen vacancy mobility is significantly reduced at either interface, with slight differences at each interface due to the differing misfit dislocation structure. Here, we conclude that if such semi-coherent oxide heterointerfaces induce enhanced ionic conductivity, it is not a consequence of higher carrier mobility.},
doi = {10.1039/C7CP04884J},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 34,
volume = 19,
place = {United States},
year = {2017},
month = {8}
}

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Works referenced in this record:

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

  • Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
  • The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
  • DOI: 10.1063/1.1329672

High Mobility in LaAlO3/SrTiO3 Heterostructures: Origin, Dimensionality, and Perspectives
journal, May 2007