Depth Profiling of Oxygen Migration in Ta/HfO2 Stacks During Ionic Liquid Gating

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Main Authors: Bednarz, Beatrice, Wortmann, Martin, Kuschel, Olga, Kammerbauer, Fabian, Kläui, Mathias, Hütten, Andreas, Wollschläger, Joachim, Jakob, Gerhard, Kuschel, Timo
Format: Preprint
Published: 2025
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author Bednarz, Beatrice
Wortmann, Martin
Kuschel, Olga
Kammerbauer, Fabian
Kläui, Mathias
Hütten, Andreas
Wollschläger, Joachim
Jakob, Gerhard
Kuschel, Timo
author_facet Bednarz, Beatrice
Wortmann, Martin
Kuschel, Olga
Kammerbauer, Fabian
Kläui, Mathias
Hütten, Andreas
Wollschläger, Joachim
Jakob, Gerhard
Kuschel, Timo
contents Ionic liquid (IL) gating has emerged as a powerful tool to control the structural, electronic, optical, and magnetic properties of materials by driving ion motion at solid interfaces. In magneto-ionic systems, electric fields are used to move ions, typically oxygen, from a donor layer into an underlying magnetic metal. Although oxygen distribution is key to enabling precise and stable control in magneto-ionic systems, the spatial distribution and voltage-dependence of oxygen incorporation in such nanoscale stacks remain unknown. Here, we quantify oxygen depth profiles and oxide formation in Si/ SiO2/ Ta (15)/ HfO2 (t) films after IL gating as a function of the gate voltage and HfO2 capping thickness (2 and 3 nm). X-ray reflectivity and X-ray photoelectron spectroscopy measurements revealed a threshold electric field of ~ -2.8 MV/cm to initiate oxygen migration from HfO2 into metallic Ta. The resulting Ta2O5 thickness increases linearly with gate voltage, reaching up to 4 nm at -3 V gating. Notably, the required electric field rises with oxide thickness, indicating a progressively growing barrier for thicker oxide films. The Ta/Ta2O5 interface remains atomically sharp for all gate voltages. This suggests that complete Ta2O5 layers form sequentially before further oxygen penetration, with no sign of deeper diffusion into bulk Ta. Thinner capping layers enhance oxidation, relevant for optimized stack design. Additionally, indium migration from the indium tin oxide electrode to the sample surface was observed, which should be considered for surface-sensitive applications. These insights advance design principles for magneto-ionic and nanoionic devices requiring precise interface engineering.
format Preprint
id arxiv_https___arxiv_org_abs_2509_05748
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Depth Profiling of Oxygen Migration in Ta/HfO2 Stacks During Ionic Liquid Gating
Bednarz, Beatrice
Wortmann, Martin
Kuschel, Olga
Kammerbauer, Fabian
Kläui, Mathias
Hütten, Andreas
Wollschläger, Joachim
Jakob, Gerhard
Kuschel, Timo
Materials Science
Mesoscale and Nanoscale Physics
Ionic liquid (IL) gating has emerged as a powerful tool to control the structural, electronic, optical, and magnetic properties of materials by driving ion motion at solid interfaces. In magneto-ionic systems, electric fields are used to move ions, typically oxygen, from a donor layer into an underlying magnetic metal. Although oxygen distribution is key to enabling precise and stable control in magneto-ionic systems, the spatial distribution and voltage-dependence of oxygen incorporation in such nanoscale stacks remain unknown. Here, we quantify oxygen depth profiles and oxide formation in Si/ SiO2/ Ta (15)/ HfO2 (t) films after IL gating as a function of the gate voltage and HfO2 capping thickness (2 and 3 nm). X-ray reflectivity and X-ray photoelectron spectroscopy measurements revealed a threshold electric field of ~ -2.8 MV/cm to initiate oxygen migration from HfO2 into metallic Ta. The resulting Ta2O5 thickness increases linearly with gate voltage, reaching up to 4 nm at -3 V gating. Notably, the required electric field rises with oxide thickness, indicating a progressively growing barrier for thicker oxide films. The Ta/Ta2O5 interface remains atomically sharp for all gate voltages. This suggests that complete Ta2O5 layers form sequentially before further oxygen penetration, with no sign of deeper diffusion into bulk Ta. Thinner capping layers enhance oxidation, relevant for optimized stack design. Additionally, indium migration from the indium tin oxide electrode to the sample surface was observed, which should be considered for surface-sensitive applications. These insights advance design principles for magneto-ionic and nanoionic devices requiring precise interface engineering.
title Depth Profiling of Oxygen Migration in Ta/HfO2 Stacks During Ionic Liquid Gating
topic Materials Science
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2509.05748