Lohaus, Katharina Natalie Silvana (2023)
Defect level identification in acceptor-doped polycrystalline barium titanate.
Technische Universität Darmstadt
doi: 10.26083/tuprints-00024453
Ph.D. Thesis, Primary publication, Publisher's Version
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Item Type: | Ph.D. Thesis | ||||
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Type of entry: | Primary publication | ||||
Title: | Defect level identification in acceptor-doped polycrystalline barium titanate | ||||
Language: | English | ||||
Referees: | Klein, Prof. Dr. Andreas ; Koruza, Prof. Dr. Jurij | ||||
Date: | 21 September 2023 | ||||
Place of Publication: | Darmstadt | ||||
Collation: | vii, 282 Seiten | ||||
Date of oral examination: | 24 July 2023 | ||||
DOI: | 10.26083/tuprints-00024453 | ||||
Abstract: | The major objective of this work is the development and qualification of two promising approaches for defect level identification in acceptor-doped polycrystalline barium titanate. To allow measurements on defined high-quality samples, undoped, Mn- and Fe-doped polycrystalline BaTiO₃ ceramics with different acceptor-doping concentrations have been synthesized via the conventional solid-state-reaction method. The influence of acceptor-doping on the microstructure and crystal structure has been investigated by means of SEM, EBSD, and XRD analysis. After exceeding a dopant-dependent threshold value, the phase fraction of the hexagonal polymorph increases with further increase in doping concentration. The appearance of the non-ferroelectric hexagonal polymorph had considerable consequences for the microstructure as well as the temperature-dependent permittivity and the ferroelectric behavior (P-E loops). The first goal of this work was to elaborate, if the defect energy levels in acceptor-doped polycrystalline BaTiO₃ can be identified using X-ray photoelectron spectroscopy. For this purpose, the Fermi level position during contact formation of RuO₂, PtOₓ, and Sn-doped In₂O₃ electrodes to polycrystalline BaTiO₃ ceramics with different Mn-doping and oxygen vacancy concentrations has been examined by means of XPS. In addition, the experimental data has been used to simulate the contact formation between RuO₂ and reduced Mn-doped BaTiO₃. The combination of experiment and simulation revealed that the interface approach is only utilizable for low-permittivity materials. The second goal of this work was to elaborate, to which extent re-oxidation experiments can be used to identify the defect energy levels in acceptor-doped polycrystalline BaTiO₃. For this purpose, Mn- and Fe-doped polycrystalline BaTiO₃ specimens have been slowly re-oxidized by temperature cycling, while the DC-conductivity was monitored. In addition, the different contributions to the electronic conductivity have been simulated using MATLAB. The comparison between simulated and experimental activation energy evolution revealed considerable differences. This indicates that the current simulation tool did not capture all effects, which contribute to the electronic conductivity. To this state, no reliable defect level identification and quantitative description of the re-oxidation experiments is possible, yet. However, the obtained results enabled a quantitative understanding of space charge region characteristics at grain boundaries. Finally, the influence of Mn- and Fe-doping on the resistance degradation of polycrystalline BaTiO₃ has been investigated. Both acceptors increased the lifetime of polycrystalline BaTiO₃, with Mn-doping being significantly more efficient than Fe-doping. |
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Status: | Publisher's Version | ||||
URN: | urn:nbn:de:tuda-tuprints-244532 | ||||
Classification DDC: | 500 Science and mathematics > 500 Science 600 Technology, medicine, applied sciences > 620 Engineering and machine engineering |
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Divisions: | 11 Department of Materials and Earth Sciences > Material Science 11 Department of Materials and Earth Sciences > Material Science > Electronic Structure of Materials (ESM) |
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Date Deposited: | 21 Sep 2023 14:26 | ||||
Last Modified: | 27 Sep 2023 08:27 | ||||
URI: | https://tuprints.ulb.tu-darmstadt.de/id/eprint/24453 | ||||
PPN: | 511904339 | ||||
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