Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman Spectroscopy
The exploitation of advanced materials for novel energy, health, and computing applications requires deep insight and fundamental understanding of physicochemical mechanisms, such as ionic and electronic conductivity, defect formation processes, and reaction kinetics. Therefore, access to the underl...
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| Format: | Article |
| Language: | English |
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Wiley-VCH
2024-11-01
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| Series: | Small Structures |
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| Online Access: | https://doi.org/10.1002/sstr.202400237 |
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| author | Alexander Stangl Nicolas Nuns Caroline Pirovano Kosova Kreka Francesco Chiabrera Albert Tarancón Mónica Burriel |
| author_facet | Alexander Stangl Nicolas Nuns Caroline Pirovano Kosova Kreka Francesco Chiabrera Albert Tarancón Mónica Burriel |
| author_sort | Alexander Stangl |
| collection | DOAJ |
| description | The exploitation of advanced materials for novel energy, health, and computing applications requires deep insight and fundamental understanding of physicochemical mechanisms, such as ionic and electronic conductivity, defect formation processes, and reaction kinetics. Therefore, access to the underlying constants of the functional materials via advanced but accessible and straightforward experimental techniques is key. Herein, a novel, cheap, fast, and widely applicable approach is presented to analyze oxygen tracer diffusion in thin films with unprecedented time resolution based on the novel in situ isotope exchange Raman spectroscopy (IERS) methodology. IERS utilizes the sensitivity of micro‐Raman spectroscopy to changes in the local isotopic composition. In‐plane tracer diffusion gradients are established by partially blocking the exchange at the surface followed by an isotope exchange. The isotope exchange and diffusion processes are followed via consecutive spatial and time‐resolved in situ Raman line scans. These isotopic gradients are analyzed to obtain mass transport coefficients, with an additional time component, not accessible by conventional destructive techniques. Diffusion coefficients of gadolinium‐doped ceria (CGO) thin films are reported within the range of interest for intermediate‐temperature emerging applications and confirm the validity of the measurement procedure and extracted parameters by comparison with the finite‐element method simulations and literature results. |
| format | Article |
| id | doaj-art-a18fe965088a445195876d9e57d0cd3c |
| institution | OA Journals |
| issn | 2688-4062 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Small Structures |
| spelling | doaj-art-a18fe965088a445195876d9e57d0cd3c2025-08-20T02:12:29ZengWiley-VCHSmall Structures2688-40622024-11-01511n/an/a10.1002/sstr.202400237Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman SpectroscopyAlexander Stangl0Nicolas Nuns1Caroline Pirovano2Kosova Kreka3Francesco Chiabrera4Albert Tarancón5Mónica Burriel6CNRS Grenoble‐INP LMGP Universite Grenoble Alpes 38000 Grenoble FranceCNRS Centrale Lille Universite d’Artois UMR 8181—UCCS—Unité de Catalyse et Chimie du Solide Universite de Lille F‐59000 Lille FranceCNRS Centrale Lille Universite d’Artois UMR 8181—UCCS—Unité de Catalyse et Chimie du Solide Universite de Lille F‐59000 Lille FranceDepartment of Advanced Materials for Energy Catalonia Institute for Energy Research (IREC) 08930 Barcelona SpainDepartment of Advanced Materials for Energy Catalonia Institute for Energy Research (IREC) 08930 Barcelona SpainDepartment of Advanced Materials for Energy Catalonia Institute for Energy Research (IREC) 08930 Barcelona SpainCNRS Grenoble‐INP LMGP Universite Grenoble Alpes 38000 Grenoble FranceThe exploitation of advanced materials for novel energy, health, and computing applications requires deep insight and fundamental understanding of physicochemical mechanisms, such as ionic and electronic conductivity, defect formation processes, and reaction kinetics. Therefore, access to the underlying constants of the functional materials via advanced but accessible and straightforward experimental techniques is key. Herein, a novel, cheap, fast, and widely applicable approach is presented to analyze oxygen tracer diffusion in thin films with unprecedented time resolution based on the novel in situ isotope exchange Raman spectroscopy (IERS) methodology. IERS utilizes the sensitivity of micro‐Raman spectroscopy to changes in the local isotopic composition. In‐plane tracer diffusion gradients are established by partially blocking the exchange at the surface followed by an isotope exchange. The isotope exchange and diffusion processes are followed via consecutive spatial and time‐resolved in situ Raman line scans. These isotopic gradients are analyzed to obtain mass transport coefficients, with an additional time component, not accessible by conventional destructive techniques. Diffusion coefficients of gadolinium‐doped ceria (CGO) thin films are reported within the range of interest for intermediate‐temperature emerging applications and confirm the validity of the measurement procedure and extracted parameters by comparison with the finite‐element method simulations and literature results.https://doi.org/10.1002/sstr.202400237functional thin filmsin situ characterizationsionic conducting oxidesoxygen tracer diffusionstime‐resolved kinetic coefficients |
| spellingShingle | Alexander Stangl Nicolas Nuns Caroline Pirovano Kosova Kreka Francesco Chiabrera Albert Tarancón Mónica Burriel Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman Spectroscopy Small Structures functional thin films in situ characterizations ionic conducting oxides oxygen tracer diffusions time‐resolved kinetic coefficients |
| title | Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman Spectroscopy |
| title_full | Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman Spectroscopy |
| title_fullStr | Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman Spectroscopy |
| title_full_unstemmed | Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman Spectroscopy |
| title_short | Real‐Time Observation of Oxygen Diffusion in CGO Thin Films Using Spatially Resolved Isotope Exchange Raman Spectroscopy |
| title_sort | real time observation of oxygen diffusion in cgo thin films using spatially resolved isotope exchange raman spectroscopy |
| topic | functional thin films in situ characterizations ionic conducting oxides oxygen tracer diffusions time‐resolved kinetic coefficients |
| url | https://doi.org/10.1002/sstr.202400237 |
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