Faster Diffusion of Oxygen Along Dislocations in (La,Sr)MnO3+δ Is a Space‐Charge Phenomenon
In displaying accelerated oxygen diffusion along extended defects, (La,Sr)MnO3+δ is an atypical acceptor‐doped perovskite‐type oxide. In this study, 18O/16O diffusion experiments on epitaxial thin films of La0.8Sr0.2MnO3+δ and molecular dynamics (MD) simulations are combined to elucidate the origin...
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Published in | Advanced functional materials Vol. 31; no. 51 |
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Abstract | In displaying accelerated oxygen diffusion along extended defects, (La,Sr)MnO3+δ is an atypical acceptor‐doped perovskite‐type oxide. In this study, 18O/16O diffusion experiments on epitaxial thin films of La0.8Sr0.2MnO3+δ and molecular dynamics (MD) simulations are combined to elucidate the origin of this phenomenon for dislocations: Does diffusion occur along dislocation cores or along space‐charge tubes? Transmission electron microscopy studies of the films revealed dislocations extending from the surface. 18O penetration profiles measured by secondary ion mass spectrometry indicated (slow) bulk diffusion and faster diffusion along dislocations. Oxygen tracer diffusivities obtained for temperatures 873 ≤ T [K] ≤ 973 were over two orders of magnitude higher for dislocations than for the bulk. The activation enthalpy of oxygen diffusion along dislocations, of (2.95 ± 0.21) eV, is surprisingly high relative to that for bulk diffusion, (2.67 ± 0.13) eV. This result militates against fast diffusion along dislocation cores. MD simulations confirmed no accelerated migration of oxide ions along dislocation cores. Faster diffusion of oxygen along dislocations in La0.8Sr0.2MnO3+δ is thus concluded to occur within space‐charge tubes in which oxygen vacancies are strongly accumulated. Reasons for and the consequences of space‐charge zones at extended defects in manganite perovskites are discussed.
A judicious combination of experimental and computational methods is used to identify the origin of faster oxygen diffusion along dislocations in the perovskite‐oxide (La,Sr)MnO3+δ. Taken together, the results from 18O diffusion experiments and molecular dynamics simulations indicate that faster diffusion cannot occur along the structural core of the dislocations but rather along enveloping space‐charge tubes. |
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AbstractList | In displaying accelerated oxygen diffusion along extended defects, (La,Sr)MnO3+δ is an atypical acceptor‐doped perovskite‐type oxide. In this study, 18O/16O diffusion experiments on epitaxial thin films of La0.8Sr0.2MnO3+δ and molecular dynamics (MD) simulations are combined to elucidate the origin of this phenomenon for dislocations: Does diffusion occur along dislocation cores or along space‐charge tubes? Transmission electron microscopy studies of the films revealed dislocations extending from the surface. 18O penetration profiles measured by secondary ion mass spectrometry indicated (slow) bulk diffusion and faster diffusion along dislocations. Oxygen tracer diffusivities obtained for temperatures 873 ≤ T [K] ≤ 973 were over two orders of magnitude higher for dislocations than for the bulk. The activation enthalpy of oxygen diffusion along dislocations, of (2.95 ± 0.21) eV, is surprisingly high relative to that for bulk diffusion, (2.67 ± 0.13) eV. This result militates against fast diffusion along dislocation cores. MD simulations confirmed no accelerated migration of oxide ions along dislocation cores. Faster diffusion of oxygen along dislocations in La0.8Sr0.2MnO3+δ is thus concluded to occur within space‐charge tubes in which oxygen vacancies are strongly accumulated. Reasons for and the consequences of space‐charge zones at extended defects in manganite perovskites are discussed. In displaying accelerated oxygen diffusion along extended defects, (La,Sr)MnO3+δ is an atypical acceptor‐doped perovskite‐type oxide. In this study, 18O/16O diffusion experiments on epitaxial thin films of La0.8Sr0.2MnO3+δ and molecular dynamics (MD) simulations are combined to elucidate the origin of this phenomenon for dislocations: Does diffusion occur along dislocation cores or along space‐charge tubes? Transmission electron microscopy studies of the films revealed dislocations extending from the surface. 18O penetration profiles measured by secondary ion mass spectrometry indicated (slow) bulk diffusion and faster diffusion along dislocations. Oxygen tracer diffusivities obtained for temperatures 873 ≤ T [K] ≤ 973 were over two orders of magnitude higher for dislocations than for the bulk. The activation enthalpy of oxygen diffusion along dislocations, of (2.95 ± 0.21) eV, is surprisingly high relative to that for bulk diffusion, (2.67 ± 0.13) eV. This result militates against fast diffusion along dislocation cores. MD simulations confirmed no accelerated migration of oxide ions along dislocation cores. Faster diffusion of oxygen along dislocations in La0.8Sr0.2MnO3+δ is thus concluded to occur within space‐charge tubes in which oxygen vacancies are strongly accumulated. Reasons for and the consequences of space‐charge zones at extended defects in manganite perovskites are discussed. A judicious combination of experimental and computational methods is used to identify the origin of faster oxygen diffusion along dislocations in the perovskite‐oxide (La,Sr)MnO3+δ. Taken together, the results from 18O diffusion experiments and molecular dynamics simulations indicate that faster diffusion cannot occur along the structural core of the dislocations but rather along enveloping space‐charge tubes. |
Author | Dittmann, Regina Weirich, Thomas E. De Souza, Roger A. Börgers, Jacqueline M. Larenz, Elizabeth Ran, Ke Kler, Joe |
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Copyright | 2021 The Authors. Advanced Functional Materials published by Wiley‐VCH GmbH 2021. This article is published under http://creativecommons.org/licenses/by-nc-nd/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. |
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Snippet | In displaying accelerated oxygen diffusion along extended defects, (La,Sr)MnO3+δ is an atypical acceptor‐doped perovskite‐type oxide. In this study, 18O/16O... |
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SubjectTerms | Defects Diffusion rate dislocations Enthalpy Manganese oxides manganite perovskite Materials science Molecular dynamics Oxygen oxygen diffusion Perovskites Secondary ion mass spectrometry Strontium Thin films Tubes |
Title | Faster Diffusion of Oxygen Along Dislocations in (La,Sr)MnO3+δ Is a Space‐Charge Phenomenon |
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