skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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:
Journal Article: 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. https://doi.org/10.1002/adts.201800095
Dholabhai, Pratik P., Martinez, Enrique, and Uberuaga, Blas P. 2018. "Influence of Chemistry and Misfit Dislocation Structure on Dopant Segregation at Complex Oxide Heterointerfaces". United States. https://doi.org/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},
url = {https://www.osti.gov/biblio/1483545}, journal = {Advanced Theory and Simulations},
issn = {2513-0390},
number = 1,
volume = 2,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

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

Save / Share:

Works referenced in this record:

All-solid-state electric-double-layer transistor based on oxide ion migration in Gd-doped CeO 2 on SrTiO 3 single crystal
journal, August 2013


Temperature Dependence Discontinuity in the Stability of Manganese-Doped Ceria Nanocrystals
journal, January 2017


Strongly enhanced oxygen ion transport through samarium-doped CeO2 nanopillars in nanocomposite films
journal, October 2015


Misfit Dislocation Guided Topographic and Conduction Patterning in Complex Oxide Epitaxial Thin Films
journal, April 2016


Shape Transitions of Epitaxial Islands during Strained Layer Growth: Anatase TiO 2 ( 001 ) on SrTiO 3 ( 001 )
journal, April 2009


Catalysis by Doped Oxides
journal, December 2012


Defect association in acceptor-doped SrTiO 3 : case study for Fe′TiV˙˙O and Mn″TiV˙˙O
journal, January 2003


Physics of SrTiO 3 -based heterostructures and nanostructures: a review
journal, February 2018


Probing dopant segregation in distinct cation sites at perovskite oxide polycrystal interfaces
journal, November 2017


Influence of acceptor doping on ionic conductivity in alkali earth titanate perovskites
journal, May 2002


Segregation of Mn 2+ Dopants as Interstitials in SrTiO 3 Grain Boundaries
journal, October 2013


Radiation Tolerant Interfaces: Influence of Local Stoichiometry at the Misfit Dislocation on Radiation Damage Resistance of Metal/Oxide Interfaces
journal, April 2017


Influence of interfacial dislocations on hysteresis loops of ferroelectric films
journal, November 2008


Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Atomic and electronic surface structures of dopants in oxides: STM and XPS of Nb- and La-doped SrTiO 3 (001)
journal, January 2011


The effects of lattice strain, dislocations, and microstructure on the transport properties of YSZ films
journal, January 2017


Solution Mechanisms for Dopant Oxides in Yttria
journal, June 1999


Colossal Ionic Conductivity at Interfaces of Epitaxial ZrO2:Y2O3/SrTiO3 Heterostructures
journal, August 2008


Magnetization in electron- and Mn- doped SrTiO3
journal, March 2013


Effect of Sintering Atmosphere on Grain Boundary Segregation and Grain Growth in Niobium-Doped SrTiO3
journal, November 2002


Theory of the Dielectric Constants of Alkali Halide Crystals
journal, October 1958


Structure and Dielectric Properties of Re 0.02 Sr 0.97 TiO 3 ( Re  = La,Sm,Gd,Er) Ceramics for High-Voltage Capacitor Applications
journal, April 2013


Structural and electronic properties of n -doped and p -doped Sr Ti O 3
journal, December 2004


Dopant Segregation and Space Charge Effects in Proton-Conducting BaZrO 3 Perovskites
journal, November 2011


Control of epitaxial relationships of ZnO/SrTiO3 heterointerfaces by etching the substrate surface
journal, January 2013


Lattice relaxation and charge-transfer optical transitions due to self-trapped holes in nonstoichiometric LaMnO3 crystal
journal, January 2002


Scale Up and Anode Development for La-Doped SrTiO 3 Anode-Supported SOFCs
journal, April 2013


Massive Interfacial Reconstruction at Misfit Dislocations in Metal/Oxide Interfaces
journal, October 2014


Stabilization of MgAl2O4 spinel surfaces via doping
journal, July 2016


Low-Temperature Ionic Conductivity of an Acceptor-Doped Perovskite: I. Impedance of Single-Crystal SrTiO 3
journal, June 2016


Electronic and Chemical Properties of a Surface-Terminated Screw Dislocation in MgO
journal, December 2013


Defect Distributions and Transport in Nanocomposites: A Theoretical Perspective
journal, July 2013


Electrical conductivity and segregation effects of doped SrTiO3 thin films
journal, January 2001


Local Structure and Energetics of Pr- and La-Doped SrTiO 3 Grain Boundaries and the Influence on Core–Shell Structure Formation
journal, October 2014


Breakthrough fuel cell technology using ceria-based multi-functional nanocomposites
journal, June 2013


Linking Interfacial Step Structure and Chemistry with Locally Enhanced Radiation-Induced Amorphization at Oxide Heterointerfaces
journal, April 2014


Structure and segregation of dopant–defect complexes at grain boundaries in nanocrystalline doped ceria
journal, January 2015


Evidence of the pressure-induced conductivity switching of yttrium-doped SrTiO 3
journal, September 2016


Orientation-specific amorphization and intercalated recrystallization at ion-irradiated SrTiO 3 /MgO interfaces
journal, August 2014


Cationic Surface Segregation in Donor-Doped SrTiO3 Under Oxidizing Conditions
journal, November 2002


Optical spectroscopy of erbium-doped SrTiO3 crystals
journal, October 2014


Dielectric measurements, Raman scattering and surface studies of Sm-doped SrTiO3 single crystal
journal, April 2010


Amphoteric doping of praseodymium Pr3+ in SrTiO3 grain boundaries
journal, March 2015


On the photoluminescence behavior of samarium-doped strontium titanate nanostructures under UV light. A structural and electronic understanding
journal, January 2010

  • Longo, Valéria Moraes; das Graça Sampaio Costa, Maria; Zirpole Simões, Alexandre
  • Physical Chemistry Chemical Physics, Vol. 12, Issue 27
  • https://doi.org/10.1039/b923281h

Role of the interface on radiation damage in the SrTiO 3 /LaAlO 3 heterostructure under Ne 2+ ion irradiation
journal, March 2014


Origin of Interface Magnetism in BiMnO 3 / SrTiO 3 and LaAlO 3 / SrTiO 3 Heterostructures
journal, August 2013


Low-Temperature Superionic Conductivity in Strained Yttria-Stabilized Zirconia
journal, May 2010


Defect cluster formation in M2O3-doped cubic ZrO2
journal, February 2000


Ionic conductivity in oxide heterostructures: the role of interfaces
journal, October 2010


Termination chemistry-driven dislocation structure at SrTiO3/MgO heterointerfaces
journal, September 2014


Radiation-induced amorphization resistance and radiation tolerance in structurally related oxides
journal, February 2007


Emergent phenomena at oxide interfaces
journal, January 2012


Interatomic potentials for strontium titanate: An assessment of their transferability and comparison with density functional theory
journal, August 2008


High-frequency electron paramagnetic resonance investigation of Mn3+ centers in SrTiO3
journal, July 2012


Interface Energies of Nanocrystalline Doped Ceria: Effects of Manganese Segregation
journal, November 2015


Segregation of xenon to dislocations and grain boundaries in uranium dioxide
journal, November 2011


On the mobility of carriers at semi-coherent oxide heterointerfaces
journal, January 2017


Cation Size Mismatch and Charge Interactions Drive Dopant Segregation at the Surfaces of Manganite Perovskites
journal, May 2013


Dopant size effects on novel functionalities: High-temperature interfacial superconductivity
journal, March 2017


Defect interactions with stepped CeO 2 /SrTiO 3 interfaces: Implications for radiation damage evolution and fast ion conduction
journal, May 2014


Die Berechnung optischer und elektrostatischer Gitterpotentiale
journal, January 1921


Monitoring the Structural and Vibrational Properties in RE-Doped SrTiO 3 Ceramic Powders
journal, July 2016


Electrical Properties of Yttrium-Doped Strontium Titanate under Reducing Conditions
journal, January 2002


Materials for Intermediate-Temperature Solid-Oxide Fuel Cells
journal, July 2014


Works referencing / citing this record:

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


Semicoherent oxide heterointerfaces: Structure, properties, and implications
journal, October 2019


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