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Title: Asymmetric Lattice Disorder Induced at Oxide Interfaces

Abstract

Control of order-disorder phase transitions is a fundamental materials science challenge, underpinning the development of energy storage technologies such as solid oxide fuel cells and batteries, ultra-high temperature ceramics, and durable nuclear waste forms. At present, the development of promising complex oxides for these applications is hindered by a poor understanding of how interfaces affect lattice disordering processes and defect transport. Here we explore the evolution of local disorder in ion-irradiated La 2Ti 2O 7/SrTiO 3 thin film heterostructures using a combination of high-resolution scanning transmission electron microscopy (STEM), position-averaged convergent beam electron diffraction (PACBED), electron energy loss spectroscopy (STEM-EELS), and ab initio theory calculations. We observe highly non-uniform lattice disordering driven by asymmetric oxygen vacancy formation across the interface. Our calculations indicate that this asymmetry results from differences in the polyhedral connectivity and vacancy formation energies of the two interface components, suggesting ways to manipulate lattice disorder in functional oxide heterostructures.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [4];  [2]
  1. Energy and Environment DirectoratePacific Northwest National Laboratory Richland WA 99352 USA
  2. Physical and Computational Sciences DirectoratePacific Northwest National Laboratory Richland WA 99352 USA
  3. Environmental Molecular Sciences LaboratoryPacific Northwest National Laboratory Richland WA 99352 USA
  4. Department of Nuclear EngineeringTexas A&,M University College Station TX 77843 USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1600867
Alternate Identifier(s):
OSTI ID: 1600871; OSTI ID: 1603102
Report Number(s):
[PNNL-SA-148989]
[Journal ID: ISSN 2196-7350]
Grant/Contract Number:  
[AC05-76RL01830]
Resource Type:
Published Article
Journal Name:
Advanced Materials Interfaces
Additional Journal Information:
[Journal Name: Advanced Materials Interfaces]; Journal ID: ISSN 2196-7350
Publisher:
Wiley-VCH
Country of Publication:
Germany
Language:
English
Subject:
ab initio; ion irradiation; order‐disorder phase transitions; oxide interfaces; thin film heterostructures

Citation Formats

Spurgeon, Steven R., Kaspar, Tiffany C., Shutthanandan, Vaithiyalingam, Gigax, Jonathan, Shao, Lin, and Sassi, Michel. Asymmetric Lattice Disorder Induced at Oxide Interfaces. Germany: N. p., 2020. Web. doi:10.1002/admi.201901944.
Spurgeon, Steven R., Kaspar, Tiffany C., Shutthanandan, Vaithiyalingam, Gigax, Jonathan, Shao, Lin, & Sassi, Michel. Asymmetric Lattice Disorder Induced at Oxide Interfaces. Germany. doi:10.1002/admi.201901944.
Spurgeon, Steven R., Kaspar, Tiffany C., Shutthanandan, Vaithiyalingam, Gigax, Jonathan, Shao, Lin, and Sassi, Michel. Thu . "Asymmetric Lattice Disorder Induced at Oxide Interfaces". Germany. doi:10.1002/admi.201901944.
@article{osti_1600867,
title = {Asymmetric Lattice Disorder Induced at Oxide Interfaces},
author = {Spurgeon, Steven R. and Kaspar, Tiffany C. and Shutthanandan, Vaithiyalingam and Gigax, Jonathan and Shao, Lin and Sassi, Michel},
abstractNote = {Control of order-disorder phase transitions is a fundamental materials science challenge, underpinning the development of energy storage technologies such as solid oxide fuel cells and batteries, ultra-high temperature ceramics, and durable nuclear waste forms. At present, the development of promising complex oxides for these applications is hindered by a poor understanding of how interfaces affect lattice disordering processes and defect transport. Here we explore the evolution of local disorder in ion-irradiated La2Ti2O7/SrTiO3 thin film heterostructures using a combination of high-resolution scanning transmission electron microscopy (STEM), position-averaged convergent beam electron diffraction (PACBED), electron energy loss spectroscopy (STEM-EELS), and ab initio theory calculations. We observe highly non-uniform lattice disordering driven by asymmetric oxygen vacancy formation across the interface. Our calculations indicate that this asymmetry results from differences in the polyhedral connectivity and vacancy formation energies of the two interface components, suggesting ways to manipulate lattice disorder in functional oxide heterostructures.},
doi = {10.1002/admi.201901944},
journal = {Advanced Materials Interfaces},
number = ,
volume = ,
place = {Germany},
year = {2020},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1002/admi.201901944

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