Formation of structural defects and strain in electrodegraded Fe-doped SrTiO3 crystals due to oxygen vacancy migration

David Ascienzo; Onur Kurt; Steve Greenbaum; Thorsten J.M. Bayer; Russell A. Maier; Clive A. Randall; Yuhang Ren

doi:10.1111/jace.15407

Formation of structural defects and strain in electrodegraded Fe-doped SrTiO₃ crystals due to oxygen vacancy migration

David Ascienzo, Onur Kurt, Steve Greenbaum, Thorsten J.M. Bayer, Russell A. Maier, Clive A. Randall, Yuhang Ren^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

21 Citations (Scopus)

Abstract

We report on our investigation of structural defect and strain formation in electrodegraded reduced and oxidized, Fe-doped SrTiO₃ (Fe:STO) single crystals using optical second harmonic generation (SHG) and confocal Raman spectroscopy. SHG and Raman spectra reveal structural and electrochemical inhomogeneity resulting from the formation of Fe⁴⁺/oxygen ion and Fe³⁺/oxygen vacancy aggregation sites along the degraded anode and cathode interfaces, respectively. We show that mixed Fe³⁺/Fe⁴⁺ states and structural strain gradients are generated across the color fronts. These results, as well as oxygen sublattice differences between the anodic and cathodic bulk, present the color front as an interface between two dominant oxygen bonding distortions. The strain near the color front shows a strong dependence on oxygen vacancy concentration and diffusion within the crystals. Our characterization of structural and electrochemical changes due to electric field-induced strain and oxygen vacancy migration advances knowledge of electrodegradation in perovskite-based titanate single crystals.

Original language	English
Pages (from-to)	2545-2561
Number of pages	17
Journal	Journal of the American Ceramic Society
Volume	101
Issue number	6
DOIs	https://doi.org/10.1111/jace.15407
Publication status	Published - Jun 2018
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2017 The American Ceramic Society

Funding

Research at Hunter was supported by an AFOSR grant (grant no. FA9550-14-1-0179 and FA9550-17-1-0339). Research at PSU was supported by an AFOSR grant (grant no. FA9550-14-1-0067).

Funders	Funder number
Air Force Office of Scientific Research	FA9550-14-1-0067, FA9550-14-1-0179, FA9550-17-1-0339

Keywords

electroceramic
oxygen vacancy
perovskite
raman spectroscopy
second harmonic generation

Access to Document

10.1111/jace.15407

Cite this

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title = "Formation of structural defects and strain in electrodegraded Fe-doped SrTiO3 crystals due to oxygen vacancy migration",

abstract = "We report on our investigation of structural defect and strain formation in electrodegraded reduced and oxidized, Fe-doped SrTiO3 (Fe:STO) single crystals using optical second harmonic generation (SHG) and confocal Raman spectroscopy. SHG and Raman spectra reveal structural and electrochemical inhomogeneity resulting from the formation of Fe4+/oxygen ion and Fe3+/oxygen vacancy aggregation sites along the degraded anode and cathode interfaces, respectively. We show that mixed Fe3+/Fe4+ states and structural strain gradients are generated across the color fronts. These results, as well as oxygen sublattice differences between the anodic and cathodic bulk, present the color front as an interface between two dominant oxygen bonding distortions. The strain near the color front shows a strong dependence on oxygen vacancy concentration and diffusion within the crystals. Our characterization of structural and electrochemical changes due to electric field-induced strain and oxygen vacancy migration advances knowledge of electrodegradation in perovskite-based titanate single crystals.",

keywords = "electroceramic, oxygen vacancy, perovskite, raman spectroscopy, second harmonic generation",

author = "David Ascienzo and Onur Kurt and Steve Greenbaum and Bayer, {Thorsten J.M.} and Maier, {Russell A.} and Randall, {Clive A.} and Yuhang Ren",

note = "Publisher Copyright: {\textcopyright} 2017 The American Ceramic Society",

year = "2018",

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T1 - Formation of structural defects and strain in electrodegraded Fe-doped SrTiO3 crystals due to oxygen vacancy migration

AU - Ascienzo, David

AU - Kurt, Onur

AU - Greenbaum, Steve

AU - Bayer, Thorsten J.M.

AU - Maier, Russell A.

AU - Randall, Clive A.

AU - Ren, Yuhang

PY - 2018/6

Y1 - 2018/6

N2 - We report on our investigation of structural defect and strain formation in electrodegraded reduced and oxidized, Fe-doped SrTiO3 (Fe:STO) single crystals using optical second harmonic generation (SHG) and confocal Raman spectroscopy. SHG and Raman spectra reveal structural and electrochemical inhomogeneity resulting from the formation of Fe4+/oxygen ion and Fe3+/oxygen vacancy aggregation sites along the degraded anode and cathode interfaces, respectively. We show that mixed Fe3+/Fe4+ states and structural strain gradients are generated across the color fronts. These results, as well as oxygen sublattice differences between the anodic and cathodic bulk, present the color front as an interface between two dominant oxygen bonding distortions. The strain near the color front shows a strong dependence on oxygen vacancy concentration and diffusion within the crystals. Our characterization of structural and electrochemical changes due to electric field-induced strain and oxygen vacancy migration advances knowledge of electrodegradation in perovskite-based titanate single crystals.

AB - We report on our investigation of structural defect and strain formation in electrodegraded reduced and oxidized, Fe-doped SrTiO3 (Fe:STO) single crystals using optical second harmonic generation (SHG) and confocal Raman spectroscopy. SHG and Raman spectra reveal structural and electrochemical inhomogeneity resulting from the formation of Fe4+/oxygen ion and Fe3+/oxygen vacancy aggregation sites along the degraded anode and cathode interfaces, respectively. We show that mixed Fe3+/Fe4+ states and structural strain gradients are generated across the color fronts. These results, as well as oxygen sublattice differences between the anodic and cathodic bulk, present the color front as an interface between two dominant oxygen bonding distortions. The strain near the color front shows a strong dependence on oxygen vacancy concentration and diffusion within the crystals. Our characterization of structural and electrochemical changes due to electric field-induced strain and oxygen vacancy migration advances knowledge of electrodegradation in perovskite-based titanate single crystals.

KW - electroceramic

KW - oxygen vacancy

KW - perovskite

KW - raman spectroscopy

KW - second harmonic generation

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