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Title: Influence of Chemistry and Misfit Dislocation Structure on Dopant Segregation at Complex Oxide Heterointerfaces

Abstract

Complex oxide heterostructures and thin films have emerged as promising candidates for diverse applications. Lattice mismatch between the two oxides lead to the formation of misfit dislocations, which influence vital material features. Trivalent dopant segregation to misfit dislocations at semi-coherent oxide heterointerfaces, while not well understood, is anticipated to impact interface-governed properties. Atomistic simulations elucidating the influence of misfit dislocations on dopant segregation at SrTiO3/MgO heterointerfaces are reported. SrO- and TiO2-terminated interfaces that have differing misfit dislocation structure were considered for trivalent dopants segregation. At SrO-terminated interface, dopants tend to segregate toward but not precisely to the heterointerface, whereas at TiO2-terminated interface, dopants exhibit a thermodynamic preference to accumulate at the heterointerface. Most favorable segregation sites at SrO-terminated interface are located within the coherent terrace, whereas those at TiO2-terminated interface are at misfit dislocation intersections. Atomic layer chemistry and the resulting misfit dislocation structure at the heterointerface, along with concomitant strain at the heterointerface due to mismatched dopants, play a critical role in influencing the observed trends for dopant segregation. Overall, the present results offer a fundamental atomic scale perspective of dopant behavior at semi-coherent complex oxide heterointerfaces and the interplay between dopant chemistry, interface chemistry, and misfit dislocation structure.

Authors:
ORCiD logo [1];  [2];  [2]
  1. Rochester Inst. of Technology, NY (United States). School of Physics and Astronomy
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rochester Inst. of Technology, NY (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); LANL Laboratory Directed Research and Development (LDRD) Program; Rochester Inst. of Technology (United States)
OSTI Identifier:
1483545
Alternate Identifier(s):
OSTI ID: 1472209
Report Number(s):
LA-UR-18-28638
Journal ID: ISSN 2513-0390
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Theory and Simulations
Additional Journal Information:
Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2513-0390
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; atomistic simulations; complex oxide heterostructures; dopant segregation; misfit dislocations; strain at heterointerfaces

Citation Formats

Dholabhai, Pratik P., Martinez, Enrique, and Uberuaga, Blas P. Influence of Chemistry and Misfit Dislocation Structure on Dopant Segregation at Complex Oxide Heterointerfaces. United States: N. p., 2018. Web. doi:10.1002/adts.201800095.
Dholabhai, Pratik P., Martinez, Enrique, & Uberuaga, Blas P. Influence of Chemistry and Misfit Dislocation Structure on Dopant Segregation at Complex Oxide Heterointerfaces. United States. doi:10.1002/adts.201800095.
Dholabhai, Pratik P., Martinez, Enrique, and Uberuaga, Blas P. Mon . "Influence of Chemistry and Misfit Dislocation Structure on Dopant Segregation at Complex Oxide Heterointerfaces". United States. doi:10.1002/adts.201800095. https://www.osti.gov/servlets/purl/1483545.
@article{osti_1483545,
title = {Influence of Chemistry and Misfit Dislocation Structure on Dopant Segregation at Complex Oxide Heterointerfaces},
author = {Dholabhai, Pratik P. and Martinez, Enrique and Uberuaga, Blas P.},
abstractNote = {Complex oxide heterostructures and thin films have emerged as promising candidates for diverse applications. Lattice mismatch between the two oxides lead to the formation of misfit dislocations, which influence vital material features. Trivalent dopant segregation to misfit dislocations at semi-coherent oxide heterointerfaces, while not well understood, is anticipated to impact interface-governed properties. Atomistic simulations elucidating the influence of misfit dislocations on dopant segregation at SrTiO3/MgO heterointerfaces are reported. SrO- and TiO2-terminated interfaces that have differing misfit dislocation structure were considered for trivalent dopants segregation. At SrO-terminated interface, dopants tend to segregate toward but not precisely to the heterointerface, whereas at TiO2-terminated interface, dopants exhibit a thermodynamic preference to accumulate at the heterointerface. Most favorable segregation sites at SrO-terminated interface are located within the coherent terrace, whereas those at TiO2-terminated interface are at misfit dislocation intersections. Atomic layer chemistry and the resulting misfit dislocation structure at the heterointerface, along with concomitant strain at the heterointerface due to mismatched dopants, play a critical role in influencing the observed trends for dopant segregation. Overall, the present results offer a fundamental atomic scale perspective of dopant behavior at semi-coherent complex oxide heterointerfaces and the interplay between dopant chemistry, interface chemistry, and misfit dislocation structure.},
doi = {10.1002/adts.201800095},
journal = {Advanced Theory and Simulations},
number = 1,
volume = 2,
place = {United States},
year = {2018},
month = {9}
}

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Cited by: 3 works
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Figures / Tables:

Figure 1 Figure 1: Structure of misfit dislocations at (a) SrO-terminated interface; (b) TiO2terminated interface. For both the cases, only interface layers are shown. View is normal to the interface. Green, blue, and yellow spheres correspond to Sr, Ti, and Mg atoms respectively. Oxygen atoms in STO are indicated by red spheres,more » whereas oxygen atoms in MgO are represented by purple spheres to offer a contrast between oxygen atoms from two different oxide phases. Misfit dislocation lines and intersections are indicated by dashed lines.« less

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    Works referencing / citing this record:

    Beyond Coherent Oxide Heterostructures: Atomic‐Scale Structure of Misfit Dislocations
    journal, June 2019

    • Dholabhai, Pratik P.; Uberuaga, Blas P.
    • Advanced Theory and Simulations, Vol. 2, Issue 9
    • DOI: 10.1002/adts.201900078

    Beyond Coherent Oxide Heterostructures: Atomic‐Scale Structure of Misfit Dislocations
    journal, June 2019

    • Dholabhai, Pratik P.; Uberuaga, Blas P.
    • Advanced Theory and Simulations, Vol. 2, Issue 9
    • DOI: 10.1002/adts.201900078

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.