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

Journal Article · · Advanced Theory and Simulations
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)

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. Here, atomistic simulations elucidating the influence of misfit dislocations on dopant segregation at SrTiO 3 /MgO heterointerfaces are reported. SrO‐ and TiO 2 ‐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 TiO 2 ‐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 TiO 2 ‐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.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Rochester Inst. of Technology, NY (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); LANL Laboratory Directed Research and Development (LDRD) Program; Rochester Inst. of Technology (United States)
Grant/Contract Number:
89233218CNA000001
OSTI ID:
1483545
Alternate ID(s):
OSTI ID: 1472209
Report Number(s):
LA-UR-18-28638
Journal Information:
Advanced Theory and Simulations, Vol. 2, Issue 1; ISSN 2513-0390
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

References (72)

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
Cu2O/TiO2 heterostructure nanotube arrays prepared by an electrodeposition method exhibiting enhanced photocatalytic activity for CO2 reduction to methanol journal February 2014
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
The classical equation of state of gaseous helium, neon and argon journal October 1938
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
  • 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
journal January 2010
δ-Doping Effects on Electronic and Energetic Properties of LaAlO 3 /SrTiO 3 Heterostructure: First-Principles Analysis of 23 Transition-Metal Dopants journal August 2017
Role of the interface on radiation damage in the SrTiO 3 /LaAlO 3 heterostructure under Ne 2+ ion irradiation journal March 2014
Self-Arranged Misfit Dislocation Network Formation upon Strain Release in La 0.7 Sr 0.3 MnO 3 /LaAlO 3 (100) Epitaxial Films under Compressive Strain journal June 2016
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
Optimization of Flux Pinning in Bulk Melt Textured 1-2-3 Superconductors: Bringing Dislocations under Control journal March 2000
Termination chemistry-driven dislocation structure at SrTiO3/MgO heterointerfaces journal September 2014
Ionic conductivity and activation energy for oxygen ion transport in superlattices—the semicoherent multilayer system YSZ (ZrO2 + 9.5 mol% Y2O3)/Y2O3 journal January 2008
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
Magnetization in electron- and Mn- doped SrTiO3 text January 2013
Physics of SrTiO$_3$-based heterostructures and nanostructures: a review text January 2017

Cited By (3)

Beyond Coherent Oxide Heterostructures: Atomic‐Scale Structure of Misfit Dislocations journal June 2019
Atomic-scale structure of misfit dislocations in CeO 2 /MgO heterostructures and thermodynamic stability of dopant–defect complexes at the heterointerface journal January 2019
Semicoherent oxide heterointerfaces: Structure, properties, and implications journal October 2019

Figures / Tables (6)