Determining the Oxygen Stoichiometry of Cobaltite Thin Films
Abstract
Transition metal oxides (TMO) are promising materials to realize low-power neuromorphic devices. Their physical properties critically depend on their oxygen vacancy concentrations, whose experimental determination remains a challenging task. Here we focus on cobaltites, in particular La1-xSrxCoO3-d (LSCO), and we present a strategy to identify fingerprints of oxygen vacancies in X-ray absorption (XA) spectra. Using a combination of experiment and theory, we show that the variation of the oxygen vacancy concentration in the perovskite phase of LSCO is correlated with the change of the relative peak positions of the O K-edge XA spectra. Furthermore, we also identify an additional geometrical fingerprint that captures both the changes of the Co-O bond length and Co-O-Co bond angle in the material due to the presence of oxygen vacancies. Finally, we predict the oxygen vacancy concentration of experimental samples and show how the resistivity of the oxide material may be tuned as a function of the defect concentration present in the system.
- Authors:
-
[1];
[3];
[2];
[6];
[3];
[2];
[8]
- Univ. of Chicago, IL (United States)
- Univ. of California, Davis, CA (United States)
- Univ. of California San Diego, La Jolla, CA (United States); Univ. of California San Diego, La Jolla, CA (United States). Center for Advanced Nanoscience
- Univ. of California San Diego, La Jolla, CA (United States)
- Purdue Univ., West Lafayette, IN (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
- Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science, Basic Energy Sciences (BES)
- OSTI Identifier:
- 1868557
- Grant/Contract Number:
- AC02-06CH11357; SC0019273; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 34; Journal Issue: 5; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; chemical structure; defects in solids; oxygen; perovskites; phase transitions
Citation Formats
Zhang, Shenli, Chiu, I-Ting, Lee, Min-Han, Gunn, Brandon, Feng, Mingzhen, Park, Tae Joon, Shafer, Padraic, N’Diaye, Alpha T., Rodolakis, Fanny, Ramanathan, Shriram, Frañó, Alex, Schuller, Ivan K., Takamura, Yayoi, and Galli, Giulia. Determining the Oxygen Stoichiometry of Cobaltite Thin Films. United States: N. p., 2022.
Web. doi:10.1021/acs.chemmater.1c03338.
Zhang, Shenli, Chiu, I-Ting, Lee, Min-Han, Gunn, Brandon, Feng, Mingzhen, Park, Tae Joon, Shafer, Padraic, N’Diaye, Alpha T., Rodolakis, Fanny, Ramanathan, Shriram, Frañó, Alex, Schuller, Ivan K., Takamura, Yayoi, & Galli, Giulia. Determining the Oxygen Stoichiometry of Cobaltite Thin Films. United States. https://doi.org/10.1021/acs.chemmater.1c03338
Zhang, Shenli, Chiu, I-Ting, Lee, Min-Han, Gunn, Brandon, Feng, Mingzhen, Park, Tae Joon, Shafer, Padraic, N’Diaye, Alpha T., Rodolakis, Fanny, Ramanathan, Shriram, Frañó, Alex, Schuller, Ivan K., Takamura, Yayoi, and Galli, Giulia. Wed .
"Determining the Oxygen Stoichiometry of Cobaltite Thin Films". United States. https://doi.org/10.1021/acs.chemmater.1c03338. https://www.osti.gov/servlets/purl/1868557.
@article{osti_1868557,
title = {Determining the Oxygen Stoichiometry of Cobaltite Thin Films},
author = {Zhang, Shenli and Chiu, I-Ting and Lee, Min-Han and Gunn, Brandon and Feng, Mingzhen and Park, Tae Joon and Shafer, Padraic and N’Diaye, Alpha T. and Rodolakis, Fanny and Ramanathan, Shriram and Frañó, Alex and Schuller, Ivan K. and Takamura, Yayoi and Galli, Giulia},
abstractNote = {Transition metal oxides (TMO) are promising materials to realize low-power neuromorphic devices. Their physical properties critically depend on their oxygen vacancy concentrations, whose experimental determination remains a challenging task. Here we focus on cobaltites, in particular La1-xSrxCoO3-d (LSCO), and we present a strategy to identify fingerprints of oxygen vacancies in X-ray absorption (XA) spectra. Using a combination of experiment and theory, we show that the variation of the oxygen vacancy concentration in the perovskite phase of LSCO is correlated with the change of the relative peak positions of the O K-edge XA spectra. Furthermore, we also identify an additional geometrical fingerprint that captures both the changes of the Co-O bond length and Co-O-Co bond angle in the material due to the presence of oxygen vacancies. Finally, we predict the oxygen vacancy concentration of experimental samples and show how the resistivity of the oxide material may be tuned as a function of the defect concentration present in the system.},
doi = {10.1021/acs.chemmater.1c03338},
journal = {Chemistry of Materials},
number = 5,
volume = 34,
place = {United States},
year = {Wed Feb 23 00:00:00 EST 2022},
month = {Wed Feb 23 00:00:00 EST 2022}
}
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