This title appears in the Scientific Report :
2020
Please use the identifier:
http://hdl.handle.net/2128/25587 in citations.
Please use the identifier: http://dx.doi.org/10.1063/5.0013965 in citations.
Cation diffusion in polycrystalline thin films of monoclinic HfO 2 deposited by atomic layer deposition
Cation diffusion in polycrystalline thin films of monoclinic HfO 2 deposited by atomic layer deposition
Though present in small amounts and migrating at low rates, intrinsic cation defects play a central role in governing the operational lifetime of oxide-ion conducting materials through slow degradation processes such as interdiffusion, kinetic demixing, grain growth, and creep. In this study, a new...
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Personal Name(s): | Mueller, Michael P. (Corresponding author) |
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Pingen, Katrin / Hardtdegen, Alexander / Aussen, Stephan / Kindsmueller, Andreas / Hoffmann-Eifert, Susanne / De Souza, Roger A. | |
Contributing Institute: |
Elektronische Materialien; PGI-7 JARA-FIT; JARA-FIT JARA Institut Green IT; PGI-10 |
Published in: | APL materials, 8 (2020) 8, S. 081104 - |
Imprint: |
Melville, NY
AIP Publ.
2020
|
DOI: |
10.1063/5.0013965 |
Document Type: |
Journal Article |
Research Program: |
Controlling Collective States |
Link: |
OpenAccess OpenAccess |
Publikationsportal JuSER |
Please use the identifier: http://dx.doi.org/10.1063/5.0013965 in citations.
Though present in small amounts and migrating at low rates, intrinsic cation defects play a central role in governing the operational lifetime of oxide-ion conducting materials through slow degradation processes such as interdiffusion, kinetic demixing, grain growth, and creep. In this study, a new experimental approach to characterizing the behavior of such slow-moving, minority defects is presented. Diffusion is probed in samples with a constant cation-defect concentration well above the equilibrium values. This approach is applied to monoclinic hafnium dioxide, m-HfO2. To this end, nanocrystalline thin films of m-HfO2 were prepared by atomic layer deposition. Diffusion experiments with ZrO2 as a diffusion source were performed in the temperature range 1173 ≤ T/K ≤ 1323 in air. The Zr diffusion profiles obtained subsequently by secondary ion mass spectrometry exhibited the following two features: the first feature was attributed to slow bulk diffusion and the second was attributed to combined fast grain-boundary diffusion and slow bulk diffusion. The activation enthalpy of Zr diffusion in bulk HfO2 was found to be (2.1 ± 0.2) eV. This result is consistent with the density-functional-theory calculations of hafnium-vacancy migration in m-HfO2, which yield values of ∼2 eV for a specific path. The activation enthalpy of the grain-boundary diffusion of (2.1 ± 0.3) eV is equal to that for bulk diffusion. This behavior is interpreted in terms of enhanced cation diffusion along space-charge layers |