Journal
MATERIALS RESEARCH BULLETIN
Volume 150, Issue -, Pages -Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.materresbull.2022.111749
Keywords
CaCu3-xMgxTi4O12; Loss tangent; Dielectric permittivity; DFT calculation; IBLC
Categories
Funding
- Fundamental Fund of Khon Kaen University
- Research and Graduate Studies Office, Khon Kaen University
- National Science, Research and Innovation Fund (NSRF)
- Khon Kaen University, Thailand
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In this study, CaCu3-xMgxTi4O12 ceramics were successfully prepared via a chemical combustion method. Mg-doped CaCu3Ti4O12 ceramics exhibited high dielectric permittivities and low loss tangents. The enhanced dielectric properties in the doped ceramics were attributed to an enhanced grain boundary response. First-principles calculations revealed the interaction between Mg atoms and the suppression of oxygen loss during the sintering process in CaCu2.90Mg0.10Ti4O12 ceramics, resulting in an increased grain boundary resistance. The internal barrier layer capacitor (IBLC) model was found to be the primary origin of the colossal dielectric response in all CaCu3-xMgxTi4O12 ceramics studied.
In this work, CaCu3-xMgxTi4O12 (x = 0, 0.05, and 0.10) ceramics were successfully prepared via a chemical combustion method. No impurity phase was detected in these two ceramics. Fine-grained microstructures were formed in all CaCu3-xMgxTi4O12 ceramics. Interestingly, high dielectric permittivities of similar to 6.58 x 10(3) - 2.87 x 10(4) with low loss tangents of similar to 0.011 - 0.025 were obtained in the Mg-doped CaCu3Ti4O12 ceramics. According to the electrical measurements, improved dielectric properties in the doped ceramic samples were a result of an enhanced grain boundary response. To elucidate the electronic structure of CaCu2.90Mg0.10Ti4O12, first-principles calculations were carried out. It was found that two Mg atoms preferentially interact. Moreover, by adding an oxygen vacancy into the CaCu2.90Mg0.10Ti4O12 structure, our results revealed that it was likely to be isolated from the Mg atoms, indicating an oxygen loss suppression during the sintering process. This resulted in an enhanced grain boundary resistance in the CaCu2.90Mg0.10Ti4O12 ceramic. Based on both the experimental and computational studies, the internal barrier layer capacitor (IBLC) model was found to be the primary origin of the colossal dielectric response in all CaCu3-xMgxTi4O12 ceramics examined in the current study.
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