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

Title: Interfacial control of oxygen vacancy doping and electrical conduction in thin film oxide heterostructures

Abstract

Oxygen vacancies in proximity to surfaces and heterointerfaces in oxide thin film heterostructures have major effects on properties, resulting, for example, in emergent conduction behavior, large changes in metal-insulator transition temperatures, or enhanced catalytic activity. Here in this paper, we report the discovery of a means of reversibly controlling the oxygen vacancy concentration and distribution in oxide heterostructures consisting of electronically conducting In2O3 films grown on ionically conducting Y2O3-stabilized ZrO2 substrates. Oxygen ion redistribution across the heterointerface is induced using an applied electric field oriented in the plane of the interface, resulting in controlled oxygen vacancy (and hence electron) doping of the film and possible orders-of-magnitude enhancement of the film's electrical conduction. The reversible modified behavior is dependent on interface properties and is attained without cation doping or changes in the gas environment.

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1352628
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Veal, Boyd W., Kim, Seong Keun, Zapol, Peter, Iddir, Hakim, Baldo, Peter M., and Eastman, Jeffrey A. Interfacial control of oxygen vacancy doping and electrical conduction in thin film oxide heterostructures. United States: N. p., 2016. Web. doi:10.1038/ncomms11892.
Veal, Boyd W., Kim, Seong Keun, Zapol, Peter, Iddir, Hakim, Baldo, Peter M., & Eastman, Jeffrey A. Interfacial control of oxygen vacancy doping and electrical conduction in thin film oxide heterostructures. United States. doi:10.1038/ncomms11892.
Veal, Boyd W., Kim, Seong Keun, Zapol, Peter, Iddir, Hakim, Baldo, Peter M., and Eastman, Jeffrey A. Fri . "Interfacial control of oxygen vacancy doping and electrical conduction in thin film oxide heterostructures". United States. doi:10.1038/ncomms11892. https://www.osti.gov/servlets/purl/1352628.
@article{osti_1352628,
title = {Interfacial control of oxygen vacancy doping and electrical conduction in thin film oxide heterostructures},
author = {Veal, Boyd W. and Kim, Seong Keun and Zapol, Peter and Iddir, Hakim and Baldo, Peter M. and Eastman, Jeffrey A.},
abstractNote = {Oxygen vacancies in proximity to surfaces and heterointerfaces in oxide thin film heterostructures have major effects on properties, resulting, for example, in emergent conduction behavior, large changes in metal-insulator transition temperatures, or enhanced catalytic activity. Here in this paper, we report the discovery of a means of reversibly controlling the oxygen vacancy concentration and distribution in oxide heterostructures consisting of electronically conducting In2O3 films grown on ionically conducting Y2O3-stabilized ZrO2 substrates. Oxygen ion redistribution across the heterointerface is induced using an applied electric field oriented in the plane of the interface, resulting in controlled oxygen vacancy (and hence electron) doping of the film and possible orders-of-magnitude enhancement of the film's electrical conduction. The reversible modified behavior is dependent on interface properties and is attained without cation doping or changes in the gas environment.},
doi = {10.1038/ncomms11892},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {6}
}

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

Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Crystal-Facet-Dependent Metallization in Electrolyte-Gated Rutile TiO 2 Single Crystals
journal, August 2013

  • Schladt, Thomas D.; Graf, Tanja; Aetukuri, Nagaphani B.
  • ACS Nano, Vol. 7, Issue 9
  • DOI: 10.1021/nn403340d

Suppression of Metal-Insulator Transition in VO2 by Electric Field-Induced Oxygen Vacancy Formation
journal, March 2013


Oxygen level: the dominant of resistive switching characteristics in cerium oxide thin films
journal, August 2012


Oxide Heterostructure Resistive Memory
journal, May 2013

  • Yang, Yuchao; Choi, ShinHyun; Lu, Wei
  • Nano Letters, Vol. 13, Issue 6
  • DOI: 10.1021/nl401287w

Magnetic effects at the interface between non-magnetic oxides
journal, June 2007

  • Brinkman, A.; Huijben, M.; van Zalk, M.
  • Nature Materials, Vol. 6, Issue 7, p. 493-496
  • DOI: 10.1038/nmat1931

Coexistence of magnetic order and two-dimensional superconductivity at LaAlO3/SrTiO3 interfaces
journal, September 2011

  • Li, Lu; Richter, C.; Mannhart, J.
  • Nature Physics, Vol. 7, Issue 10, p. 762-766
  • DOI: 10.1038/nphys2080

Emerging magnetism and electronic phase separation at titanate interfaces
journal, November 2013


Magnetic and superconducting phases at the LaAlO 3 /SrTiO 3 interface: The role of interfacial Ti 3 d electrons
journal, January 2012


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


Consequences of Oxygen-Vacancy Correlations at the SrTiO 3 Interface
journal, October 2014


Enhancement of Oxygen Surface Exchange at the Hetero-interface of (La,Sr)CoO[sub 3]/(La,Sr)[sub 2]CoO[sub 4] with PLD-Layered Films
journal, January 2008

  • Sase, M.; Hermes, F.; Yashiro, K.
  • Journal of The Electrochemical Society, Vol. 155, Issue 8
  • DOI: 10.1149/1.2928612

Orienting Oxygen Vacancies for Fast Catalytic Reaction
journal, October 2013

  • Jeen, Hyoungjeen; Bi, Zhonghe; Choi, Woo Seok
  • Advanced Materials, Vol. 25, Issue 44
  • DOI: 10.1002/adma.201302919

Electronic Activation of Cathode Superlattices at Elevated Temperatures - Source of Markedly Accelerated Oxygen Reduction Kinetics
journal, May 2013


New Insights into the Strain Coupling to Surface Chemistry, Electronic Structure, and Reactivity of La 0.7 Sr 0.3 MnO 3
journal, March 2011

  • Jalili, Helia; Han, Jeong Woo; Kuru, Yener
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 7
  • DOI: 10.1021/jz200160b

Surface strontium enrichment on highly active perovskites for oxygen electrocatalysis in solid oxide fuel cells
journal, January 2012

  • Crumlin, Ethan J.; Mutoro, Eva; Liu, Zhi
  • Energy & Environmental Science, Vol. 5, Issue 3
  • DOI: 10.1039/c2ee03397f

A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004


Metallic and Insulating Interfaces of Amorphous SrTiO 3 -Based Oxide Heterostructures
journal, September 2011

  • Chen, Yunzhong; Pryds, Nini; Kleibeuker, Josée E.
  • Nano Letters, Vol. 11, Issue 9
  • DOI: 10.1021/nl201821j

Surface defects and conduction in polar oxide heterostructures
journal, May 2011


Control of synaptic vesicle endocytosis by an extracellular signalling molecule
journal, September 2013

  • Smillie, Karen J.; Pawson, Jonathan; Perkins, Emma M.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3394

Nucleation of islands and continuous high-quality In2O3(001) films during plasma-assisted molecular beam epitaxy on Y-stabilized ZrO2(001)
journal, June 2010

  • Bierwagen, Oliver; Speck, James S.
  • Journal of Applied Physics, Vol. 107, Issue 11
  • DOI: 10.1063/1.3415539

Growth of In2O3(100) on Y-stabilized ZrO2(100) by O-plasma assisted molecular beam epitaxy
journal, March 2008

  • Bourlange, A.; Payne, D. J.; Egdell, R. G.
  • Applied Physics Letters, Vol. 92, Issue 9
  • DOI: 10.1063/1.2889500

Investigation of the growth of In2O3 on Y-stabilized ZrO2(100) by oxygen plasma assisted molecular beam epitaxy
journal, June 2009


Intrinsic n -Type Behavior in Transparent Conducting Oxides: A Comparative Hybrid-Functional Study of In 2 O 3 , SnO 2 , and ZnO
journal, December 2009


Electrical conductivity and ionic transport number of YSZ and Cr-doped YSZ single crystals at 200–1000°C
journal, December 1993


On the variability of oxygen exchange kinetics of platinum model electrodes on yttria stabilized zirconia
journal, October 2013


Charge storage at the Pt/YSZ interface
journal, November 2007

  • Fóti, György; Jaccoud, Arnaud; Falgairette, Cyril
  • Journal of Electroceramics, Vol. 23, Issue 2-4
  • DOI: 10.1007/s10832-007-9352-7

Oxygen storage in O2/Pt/YSZ cell
journal, August 2009


In situ characterization of the formation of a mixed conducting phase on the surface of yttria-stabilized zirconia near Pt electrodes
journal, September 2015


Schottky contacts to In 2 O 3
journal, April 2014

  • von Wenckstern, H.; Splith, D.; Schmidt, F.
  • APL Materials, Vol. 2, Issue 4
  • DOI: 10.1063/1.4870536

Electrical Conductivity of Silver Sulfide
journal, January 1952

  • Hebb, Malcolm H.
  • The Journal of Chemical Physics, Vol. 20, Issue 1
  • DOI: 10.1063/1.1700165

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992


Projector augmented-wave method
journal, December 1994


Ab initio prediction of ordered ground-state structures in ZrO 2 -Y 2 O 3
journal, April 2008


    Works referencing / citing this record:

    Enhancing the triiodide reduction activity of a perovskite-based electrocatalyst for dye-sensitized solar cells through exsolved silver nanoparticles
    journal, January 2019

    • Xu, Meigui; Wang, Wei; Zhong, Yijun
    • Journal of Materials Chemistry A, Vol. 7, Issue 29
    • DOI: 10.1039/c9ta05005a

    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

    Enhancing the triiodide reduction activity of a perovskite-based electrocatalyst for dye-sensitized solar cells through exsolved silver nanoparticles
    journal, January 2019

    • Xu, Meigui; Wang, Wei; Zhong, Yijun
    • Journal of Materials Chemistry A, Vol. 7, Issue 29
    • DOI: 10.1039/c9ta05005a