(Invited) Modification of Dielectric Properties of Film Dielectric Materials by Solid Solution System
Authors: Nagata Takahiro 
Published: August 2024

Compound semiconductor based power devices such as SiC and GaN require high temperature operating passive devices such as a capacitor. SiC-based active devices can operate above 250 °C. The development of high-temperature operational passives is urgently needed to advance to the module and system level. In the case of capacitors, currently available capacitors can only operate efficiently up to 175 °C. Therefore, a thin film capacitor that can operate at high temperatures and be monolithically integrated near the active device should be developed. In this talk, I will present our achievements in the development of high-temperature operating dielectric film materials using the solid solution system.
One topic is A2B2O7 pyrochlore ferroelectrics. The ferroelectric materials with the pyrochlore structure such as Sr2Nb2O7 exhibited the high dielectric constant above 100 at high and low temperature ranges. However, due to the crystallographic direction dependence of the Curie-Weiss temperature, the temperature stability of the dielectric constant from room temperature to 300 °C was not available. In order to obtain the high temperature stability of dielectric constant from room temperature to 300 °C with high dielectric constant over 100, the pyrochlore ferroelectric solid solution thin films were investigated by employing the combinatorial synthesis. Composition spread thin films of solid solution of two or three kinds of materials were deposited on substrates by physical vapor deposition technique, which provided the systematic physical properties. High-throughput combinatorial synthesis method is effective in the rapid optimization of the correlation between the crystallization and the dielectric property change behavior. For the composition spread solid solution film, the Sr- or La-containing A2B2O7 pyrochlore ferroelectrics were selected from the viewpoints of ion radios and crystallographic direction dependence of the Curie-Weiss temperature.
The composition spread films were formed on a Pt/Ti/SiO2/Si substrate by combinatorial RF sputtering with stoichiometric composition targets. The X-ray fluorescence spectrum of the composition-spread film showed a linear variation of the metal composition. After deposition, the samples were annealed at different temperatures under oxygen atmosphere to reduce oxygen vacancies and improve crystallinity. The crystallization of the composition-spread solid solution thin film was confirmed by X-ray diffraction patterns, indicating the composition dependence of the crystallographic orientation. Some compositions showed high dielectric constant over 100 and high temperature stability from room temperature to 300 °C. In the presentation, the correlation between film composition, orientation and dielectric constant will be discussed in detail.
In the presentation, we also introduce our achievement of the BaTiO3 based relaxor ferroelectrics and other dielectric materials development using the solid solution system. For the relaxor ferroelectrics, among the BaTiO3 based relaxor ferroelectrics, we have selected x[BaTiO3]-(1-x)[Bi(Mg2/3Nb1/3)O3] . The permittivity of 400 and the stability <8% from room temperature to 400 °C were obtained, which are promising as high-temperature dielectric medium.