In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films

Buckner, Haley B.; Perry, Nicola H.

doi:10.1002/admi.201900496

Title: In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films

Abstract

The authors discuss the use of in situ optical absorption to probe point defect equilibria and kinetics in oxides, with particular attention to thin films and high-temperature measurements evaluating changes in oxygen content. The introduction notes the effect of point defects on oxide behavior, including differences in thin films versus bulk materials, and describes methods to evaluate point defect equilibria and kinetics; advantages of optical absorption among these methods are highlighted. Section 2 provides an overview of how optical absorption and point defect concentrations are related, including various possible structural and electronic origins of defect-mediated absorption changes corresponding to oxygen content changes. Section 3 traces the development of historical understanding of optical absorption in nonstoichiometric oxides and emergence of thin film applications and measurement approaches that resulted. Section 4 details the procedure for determining surface exchange coefficients from optical transmission relaxation measurements and provides specific examples of how this approach uniquely has enabled new insights into thin film surface exchange behavior with and without current collectors. Section 5 provides examples of optically derived diffusivity measurements and comparisons of bulk and thin film defect equilibria. Section 7 outlines potential opportunities and future developments in this area, and Section 7 concludes themore » manuscript.« less

Authors:

Buckner, Haley B. ^[1];

^[1]

Univ. of Illinois at Urbana-Champaign, IL (United States)

Publication Date:: Mon Jul 08 00:00:00 EDT 2019

Research Org.:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1599746

Alternate Identifier(s):: OSTI ID: 1532421

Grant/Contract Number:: SC0018963

Resource Type:: Accepted Manuscript

Journal Name:: Advanced Materials Interfaces

Additional Journal Information:: Journal Volume: 6; Journal Issue: 15; Journal ID: ISSN 2196-7350

Publisher:: Wiley-VCH

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; diffusion; high‐temperature materials; nonstoichiometry; optical absorption; point defects; surface exchange kinetics; thin films

Citation Formats


                    Buckner, Haley B., and Perry, Nicola H. In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films.  United States: N. p., 2019. 
Web.  doi:10.1002/admi.201900496.

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                    Buckner, Haley B., & Perry, Nicola H. In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films.  United States.  https://doi.org/10.1002/admi.201900496

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                    Buckner, Haley B., and Perry, Nicola H. Mon .  
"In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films".  United States.  https://doi.org/10.1002/admi.201900496.  https://www.osti.gov/servlets/purl/1599746.

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@article{osti_1599746,

  title        = {In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films},

  author       = {Buckner, Haley B. and Perry, Nicola H.},

  abstractNote = {The authors discuss the use of in situ optical absorption to probe point defect equilibria and kinetics in oxides, with particular attention to thin films and high-temperature measurements evaluating changes in oxygen content. The introduction notes the effect of point defects on oxide behavior, including differences in thin films versus bulk materials, and describes methods to evaluate point defect equilibria and kinetics; advantages of optical absorption among these methods are highlighted. Section 2 provides an overview of how optical absorption and point defect concentrations are related, including various possible structural and electronic origins of defect-mediated absorption changes corresponding to oxygen content changes. Section 3 traces the development of historical understanding of optical absorption in nonstoichiometric oxides and emergence of thin film applications and measurement approaches that resulted. Section 4 details the procedure for determining surface exchange coefficients from optical transmission relaxation measurements and provides specific examples of how this approach uniquely has enabled new insights into thin film surface exchange behavior with and without current collectors. Section 5 provides examples of optically derived diffusivity measurements and comparisons of bulk and thin film defect equilibria. Section 7 outlines potential opportunities and future developments in this area, and Section 7 concludes the manuscript.},

  doi          = {10.1002/admi.201900496},

  journal      = {Advanced Materials Interfaces},

  number       = 15,

  volume       = 6,

  place        = {United States},

  year         = {Mon Jul 08 00:00:00 EDT 2019},

  month        = {Mon Jul 08 00:00:00 EDT 2019}

}

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Figure 1: (a)-(c) show the color changes associated with an increase in growth temperature in SrTi_0.65Fe_0.35O_3-δ thin films. Adapted from Ref. [69] with permission from The Royal Society of Chemistry. (d)-(f) show the color changes associated with increasing pO₂ in Sr_1-xLaxTi_1-yFeyO_3-δ thin films. Adapted with permission from N.H. Perry, N.more »

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Perry, Nicola H.; Kim, Jae Jin; Tuller, Harry L.
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Investigation of Nonstoichiometry in Oxide Thin Films by Simultaneous in Situ Optical Absorption and Chemical Capacitance Measurements: Pr-Doped Ceria, a Case Study
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Kim, Jae Jin; Bishop, Sean R.; Thompson, Nicholas J.
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Figures / Tables found in this record:

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Solid-state heterointerfaces are of interest for emergent local behavior that is distinct from either bulk parent compound. One technologically relevant example is the case of mixed ionic/electronic conductor (MIEC)–metal interfaces, which play an important role in electrochemistry. Metal–MIEC composite electrodes can demonstrate improved catalytic activity vs single-phase MIECs, improving fuel cell efficiency. Similarly, MIEC surface reaction kinetics are often evaluated using techniques that place metal current collectors in contact with the surface under evaluation, potentially altering the response vs the native surface. Here, techniques enabling direct and local in situ observation of the behavior at and around such heterointerfaces aremore »« less
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Title: In Situ Optical Absorption Studies of Point Defect Kinetics and Thermodynamics in Oxide Thin Films

Abstract

Citation Formats

Figures / Tables:

Photochromism in Transition-Metal-Doped SrTi O 3 journal, November 1971

Non-equilibrium origin of high electrical conductivity in gallium zinc oxide thin films journal, December 2013

The interplay and impact of strain and defect association on the conductivity of rare-earth substituted ceria journal, March 2019

Practical considerations for reliable stress and oxygen surface exchange coefficients from bilayer curvature relaxation measurements journal, December 2016

Chemical expansion of praseodymium-cerium oxide films at high temperatures by laser doppler vibrometry journal, June 2018

Electrical conductivity and defect equilibria of Pr0.1Ce0.9O2−δ journal, January 2011

Temperature Dependence of Effective Grain Core/Single Crystal Dielectric Constants for Acceptor-Doped Oxygen Ion Conductors: Temperature Dependence of Effective Grain Core/Single Crystal Dielectric Constants journal, September 2010

Photochromism of metal oxides—I the light sensitivity of MoO3 or WO3 coprecipitated with TiO2 journal, January 1966

Band gap engineered TiO 2 nanoparticles for visible light induced photoelectrochemical and photocatalytic studies journal, January 2014

Impedance Spectroscopy: Theory, Experiment, and Applications book, March 2018

ESR and optical absorption of bound-small polarons in YAl O 3 journal, June 1975

Equilibrium Electrical Property Measurements in Electroceramics journal, October 1996

Mass Transport in Oxide Thin Films - Visualization and Control journal, September 2015

Influence of Minor Additions on Color and Electrical Properties of Rutile journal, December 1949

Tracer diffusion and chemical diffusion of oxygen in acceptor doped SrTiO 3 journal, August 2000

Relating Microstructure to Surface Exchange Kinetics Using in Situ Optical Absorption Relaxation journal, January 2017

Defects and transport in complex oxide thin films journal, May 2008

Impedance Spectroscopy as a Tool for Chemical and Electrochemical Analysis of Mixed Conductors: A Case Study of Ceria journal, November 2005

Anderson transition and intermediate polaron formation in WO 3-x Transport properties and optical absorption journal, November 1984

X-ray absorption and dichroism of transition metals and their compounds journal, August 1994

Understanding chemical expansion in perovskite-structured oxides journal, January 2015

On the Electrochromism of Evaporated V 2 O 5 Films journal, August 1985

The electronic structure of β-Ga2O3 journal, November 2010

Combined Tip-Enhanced Raman Spectroscopy and Scattering-Type Scanning Near-Field Optical Microscopy journal, June 2018

Fast scanning spectroelectrochemical ellipsometry: In-situ characterization of gold oxide journal, July 1990

Kinetics and Mechanisms of Oxygen Surface Exchange on La[sub 0.6]Sr[sub 0.4]FeO[sub 3−δ] Thin Films journal, January 2009

Use of the quartz crystal microbalance to measure the mass of submonolayer deposits: Measuring the stoichiometry of surface oxides journal, May 1998

Photochromic effect in impurity-doped PLZT ceramics journal, January 1974

Electrode influence on the charge transport through SrTiO 3 thin films journal, November 1995

Local electrical and dielectric properties of nanocrystalline yttria-stabilized zirconia journal, July 2008

Mossbauer evidence for hole trapping by ferric acceptor states on rutile surfaces journal, October 1972

Nanograin Composite Model Studies of Nanocrystalline Gadolinia-Doped Ceria: Nanograin Composite Model Studies journal, November 2010

Surface and bulk electrical properties of the hematite phase Fe2O3 journal, October 1991

Investigation of Redox Kinetics by Simultaneous In Situ Optical Absorption Relaxation and Electrode Impedance Measurements: Pr Doped Ceria Thin Films journal, October 2013

Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects journal, February 2015

Some Solid‐State Studies of Tungsten Trioxide and Their Significance to Tungsten Bronze Theory journal, April 1963

Grain core and grain boundary electrical/dielectric properties of yttria-doped tetragonal zirconia polycrystal (TZP) nanoceramics journal, March 2010

Electronic Processes in Ionic Crystals (Mott, N. F.; Gurney, R. W.) journal, May 1941

Characterisation of La0.6Sr0.4Co0.2Fe0.8O3-d and Ba0.5Sr0.5Co0.8Fe0.2O3-d as Cathode Materials for the Application in Intermediate Temperature Fuel Cells conference, January 2007

An Optical In-Situ Method to Study Redox-Kinetics in SrTiO3 journal, September 1993

High-temperature ligand field spectra and cation disorder and dynamics in spinels: CoAl2O4 journal, September 1988

Raman Spectrum of Alumina and the Luminescence and Absorption Spectra of Ruby journal, July 1947

Confirmation of the Dominant Defect Mechanism in Amorphous In-Zn-O Through the Application of In Situ Brouwer Analysis journal, April 2015

Chemical Expansivity of Electrochemical Ceramics journal, September 2001

Enhancement of oxygen surface kinetics of SrTiO3 by alkaline earth metal oxides journal, October 2006

A Novel Electrophotographic System journal, January 1969

Valence states of iron in photochromic strontium titanate by Mössbauer effect journal, August 1973

Origin and Tunability of Unusually Large Surface Capacitance in Doped Cerium Oxide Studied by Ambient-Pressure X-Ray Photoelectron Spectroscopy journal, March 2016

Color Centers in Alkali Halide Crystals. II journal, January 1954

Origins and Control of Optical Absorption in a Nondilute Oxide Solid Solution: Sr(Ti,Fe)O 3– x Perovskite Case Study journal, January 2019

Point Defects in Oxides: Tailoring Materials Through Defect Engineering journal, August 2011

Free-carrier plasma resonance effects and electron transport in reactively sputtered degenerate ZnO:Al films journal, March 1999

Defect chemistry and surface oxygen exchange kinetics of La-doped Sr(Ti,Fe)O3− in oxygen-rich atmospheres journal, May 2015

III. Spin resonance studies of defects in magnesium oxide journal, January 1959

Defect spectroscopy with positrons: a general calculational method journal, February 1983

Oxygen transport in La0.6Sr0.4Co1−y Fe y O3−δ journal, March 2004

Decontamination and disinfection of water by solar photocatalysis: The pilot plants of the Plataforma Solar de Almeria journal, February 2016

Treatment of the Impedance of Mixed Conductors Equivalent Circuit Model and Explicit Approximate Solutions journal, January 1999

Modulated and ordered defect structures in electrically degraded Ni–BaTiO3 multilayer ceramic capacitors journal, November 2003

Improved chemical and electrochemical stability of perovskite oxides with less reducible cations at the surface journal, June 2016

Jahn-Teller distortion around Fe 4 + in Sr ( Fe x Ti 1 − x ) O 3 − δ from x-ray absorption spectroscopy, x-ray diffraction, and vibrational spectroscopy journal, November 2007

Raman spectroscopy of molybdenum oxides journal, January 2002

Photochromism and electrochromism in amorphous transition metal oxide films journal, April 1978

Structural Studies of Tin-Doped Indium Oxide (ITO) and In4Sn3O12 journal, January 1998

Empirical in operando analysis of the charge carrier dynamics in hematite photoanodes by PEIS, IMPS and IMVS journal, January 2016

Oxygen Surface Exchange Kinetics on Sr-Substituted Lanthanum Manganite and Ferrite Thin-Film Microelectrodes journal, January 2009

The valence change of Fe in BaTiO3 studied by Mössbauer effect and gravimetry journal, September 1980

Grain boundary resistivity in zirconia-based materials: effect of sintering temperatures and impurities journal, February 1995

In situ photoacoustic spectroscopy of thin oxide layers on metal electrodes. Copper in alkaline solution journal, February 1981

Electron Spin Resonance of F Centers in Magnesium Oxide; Confirmation of the Spin of Magnesium-25 journal, September 1957

Thermal and Chemical Expansion of Sr-Doped Lanthanum Cobalt Oxide (La 1 - x Sr x CoO 3 - δ ) journal, August 2005

Comparison of oxygen exchange kinetics of the IT-SOFC cathode materials La0.5Sr0.5CoO3−δ and La0.6Sr0.4CoO3−δ journal, October 2012

In situ oxygen surface exchange coefficient measurements on lanthanum strontium ferrite thin films via the curvature relaxation method journal, November 2013

Surface exchange of oxygen in mixed conducting perovskite oxides journal, July 1996

Coupling of strain, stress, and oxygen non-stoichiometry in thin film Pr 0.1 Ce 0.9 O 2−δ journal, January 2016

Memristor Kinetics and Diffusion Characteristics for Mixed Anionic-Electronic SrTiO 3-δ Bits: The Memristor-Based Cottrell Analysis Connecting Material to Device Performance journal, September 2014

Photochromism in Transition-Metal-Doped SrTi $O_{3}$
journal, November 1971

Non-equilibrium origin of high electrical conductivity in gallium zinc oxide thin films
journal, December 2013

The interplay and impact of strain and defect association on the conductivity of rare-earth substituted ceria
journal, March 2019

Practical considerations for reliable stress and oxygen surface exchange coefficients from bilayer curvature relaxation measurements
journal, December 2016

Chemical expansion of praseodymium-cerium oxide films at high temperatures by laser doppler vibrometry
journal, June 2018

Electrical conductivity and defect equilibria of Pr0.1Ce0.9O2−δ
journal, January 2011

Temperature Dependence of Effective Grain Core/Single Crystal Dielectric Constants for Acceptor-Doped Oxygen Ion Conductors: Temperature Dependence of Effective Grain Core/Single Crystal Dielectric Constants
journal, September 2010

Photochromism of metal oxides—I the light sensitivity of MoO3 or WO3 coprecipitated with TiO2
journal, January 1966

Band gap engineered TiO ₂ nanoparticles for visible light induced photoelectrochemical and photocatalytic studies
journal, January 2014

Impedance Spectroscopy: Theory, Experiment, and Applications
book, March 2018

ESR and optical absorption of bound-small polarons in YAl $O_{3}$
journal, June 1975

Equilibrium Electrical Property Measurements in Electroceramics
journal, October 1996

Mass Transport in Oxide Thin Films - Visualization and Control
journal, September 2015

Influence of Minor Additions on Color and Electrical Properties of Rutile
journal, December 1949

Tracer diffusion and chemical diffusion of oxygen in acceptor doped SrTiO 3
journal, August 2000

Relating Microstructure to Surface Exchange Kinetics Using in Situ Optical Absorption Relaxation
journal, January 2017

Defects and transport in complex oxide thin films
journal, May 2008

Impedance Spectroscopy as a Tool for Chemical and Electrochemical Analysis of Mixed Conductors: A Case Study of Ceria
journal, November 2005

Anderson transition and intermediate polaron formation in WO _3-x Transport properties and optical absorption
journal, November 1984

X-ray absorption and dichroism of transition metals and their compounds
journal, August 1994

Understanding chemical expansion in perovskite-structured oxides
journal, January 2015

On the Electrochromism of Evaporated V ₂ O ₅ Films
journal, August 1985

The electronic structure of β-Ga2O3
journal, November 2010

Combined Tip-Enhanced Raman Spectroscopy and Scattering-Type Scanning Near-Field Optical Microscopy
journal, June 2018

Fast scanning spectroelectrochemical ellipsometry: In-situ characterization of gold oxide
journal, July 1990

Kinetics and Mechanisms of Oxygen Surface Exchange on La[sub 0.6]Sr[sub 0.4]FeO[sub 3−δ] Thin Films
journal, January 2009

Use of the quartz crystal microbalance to measure the mass of submonolayer deposits: Measuring the stoichiometry of surface oxides
journal, May 1998

Photochromic effect in impurity-doped PLZT ceramics
journal, January 1974

Electrode influence on the charge transport through SrTiO ₃ thin films
journal, November 1995

Local electrical and dielectric properties of nanocrystalline yttria-stabilized zirconia
journal, July 2008

Mossbauer evidence for hole trapping by ferric acceptor states on rutile surfaces
journal, October 1972

Nanograin Composite Model Studies of Nanocrystalline Gadolinia-Doped Ceria: Nanograin Composite Model Studies
journal, November 2010

Surface and bulk electrical properties of the hematite phase Fe2O3
journal, October 1991

Investigation of Redox Kinetics by Simultaneous In Situ Optical Absorption Relaxation and Electrode Impedance Measurements: Pr Doped Ceria Thin Films
journal, October 2013

Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects
journal, February 2015

Some Solid‐State Studies of Tungsten Trioxide and Their Significance to Tungsten Bronze Theory
journal, April 1963

Grain core and grain boundary electrical/dielectric properties of yttria-doped tetragonal zirconia polycrystal (TZP) nanoceramics
journal, March 2010

Electronic Processes in Ionic Crystals (Mott, N. F.; Gurney, R. W.)
journal, May 1941

Characterisation of La0.6Sr0.4Co0.2Fe0.8O3-d and Ba0.5Sr0.5Co0.8Fe0.2O3-d as Cathode Materials for the Application in Intermediate Temperature Fuel Cells
conference, January 2007

An Optical In-Situ Method to Study Redox-Kinetics in SrTiO3
journal, September 1993

High-temperature ligand field spectra and cation disorder and dynamics in spinels: CoAl2O4
journal, September 1988

Raman Spectrum of Alumina and the Luminescence and Absorption Spectra of Ruby
journal, July 1947

Confirmation of the Dominant Defect Mechanism in Amorphous In-Zn-O Through the Application of In Situ Brouwer Analysis
journal, April 2015

Chemical Expansivity of Electrochemical Ceramics
journal, September 2001

Enhancement of oxygen surface kinetics of SrTiO3 by alkaline earth metal oxides
journal, October 2006

A Novel Electrophotographic System
journal, January 1969

Valence states of iron in photochromic strontium titanate by Mössbauer effect
journal, August 1973

Origin and Tunability of Unusually Large Surface Capacitance in Doped Cerium Oxide Studied by Ambient-Pressure X-Ray Photoelectron Spectroscopy
journal, March 2016

Color Centers in Alkali Halide Crystals. II
journal, January 1954

Origins and Control of Optical Absorption in a Nondilute Oxide Solid Solution: Sr(Ti,Fe)O _{3– x} Perovskite Case Study
journal, January 2019

Point Defects in Oxides: Tailoring Materials Through Defect Engineering
journal, August 2011

Free-carrier plasma resonance effects and electron transport in reactively sputtered degenerate ZnO:Al films
journal, March 1999

Defect chemistry and surface oxygen exchange kinetics of La-doped Sr(Ti,Fe)O3− in oxygen-rich atmospheres
journal, May 2015

III. Spin resonance studies of defects in magnesium oxide
journal, January 1959

Defect spectroscopy with positrons: a general calculational method
journal, February 1983

Oxygen transport in La0.6Sr0.4Co1−y Fe y O3−δ
journal, March 2004

Decontamination and disinfection of water by solar photocatalysis: The pilot plants of the Plataforma Solar de Almeria
journal, February 2016

Treatment of the Impedance of Mixed Conductors Equivalent Circuit Model and Explicit Approximate Solutions
journal, January 1999

Modulated and ordered defect structures in electrically degraded Ni–BaTiO3 multilayer ceramic capacitors
journal, November 2003

Improved chemical and electrochemical stability of perovskite oxides with less reducible cations at the surface
journal, June 2016

Jahn-Teller distortion around ${Fe}^{4 +}$ in $Sr ({Fe}_{x} {Ti}_{1 - x}) O_{3 - δ}$ from x-ray absorption spectroscopy, x-ray diffraction, and vibrational spectroscopy
journal, November 2007

Raman spectroscopy of molybdenum oxides
journal, January 2002

Photochromism and electrochromism in amorphous transition metal oxide films
journal, April 1978

Structural Studies of Tin-Doped Indium Oxide (ITO) and In4Sn3O12
journal, January 1998

Empirical in operando analysis of the charge carrier dynamics in hematite photoanodes by PEIS, IMPS and IMVS
journal, January 2016

Oxygen Surface Exchange Kinetics on Sr-Substituted Lanthanum Manganite and Ferrite Thin-Film Microelectrodes
journal, January 2009

The valence change of Fe in BaTiO3 studied by Mössbauer effect and gravimetry
journal, September 1980

Grain boundary resistivity in zirconia-based materials: effect of sintering temperatures and impurities
journal, February 1995

In situ photoacoustic spectroscopy of thin oxide layers on metal electrodes. Copper in alkaline solution
journal, February 1981

Electron Spin Resonance of $F$ Centers in Magnesium Oxide; Confirmation of the Spin of Magnesium-25
journal, September 1957

Thermal and Chemical Expansion of Sr-Doped Lanthanum Cobalt Oxide (La ₁ _- _x Sr _x CoO ₃ _- _δ )
journal, August 2005

Comparison of oxygen exchange kinetics of the IT-SOFC cathode materials La0.5Sr0.5CoO3−δ and La0.6Sr0.4CoO3−δ
journal, October 2012

In situ oxygen surface exchange coefficient measurements on lanthanum strontium ferrite thin films via the curvature relaxation method
journal, November 2013

Surface exchange of oxygen in mixed conducting perovskite oxides
journal, July 1996

Coupling of strain, stress, and oxygen non-stoichiometry in thin film Pr _0.1 Ce _0.9 O _2−δ
journal, January 2016

Memristor Kinetics and Diffusion Characteristics for Mixed Anionic-Electronic SrTiO _3-δ Bits: The Memristor-Based Cottrell Analysis Connecting Material to Device Performance
journal, September 2014

Photochromism in Ni-doped SrTi $O_{3}$
journal, October 1976

Enhancing Perovskite Electrocatalysis through Strain Tuning of the Oxygen Deficiency
journal, June 2016

Real-time impedance monitoring of oxygen reduction during surface modification of thin film cathodes
journal, March 2017

Measuring oxygen diffusion and oxygen surface exchange by conductivity relaxation
journal, November 2000