Radio frequency (rf) atmospheric pressure glow discharges (APGDs) have received growing attention for their exciting scope of new science and their immense potential for widespread applications. While geometrically similar to conventional low-pressure discharges used in the semiconductor industry for decades, rf APGDs present new physics that require investigation. This thesis presents an experimental and computational study of helium rfAPGDs aimed at making a contribution to the current understanding of these discharges and enabling their optimization for different applications. The timely interest and significance of this work is highlighted by the publication of different parts of this thesis in 10 peer-reviewed international journals. Starting with the electron trapping in rf APGDs, the thesis looks into the electron heating mechanism responsible for sustaining the discharges, the influence of the rf excitation frequency on the discharge characteristics, the role of impurities in the discharge chemistry as well as the evolution of the discharge as the size is reduced down to microplasma dimensions. The findings of this research are based on the synergistic use of electrical measurements, optical diagnostics and self-developed computational models. With the knowledge gained from this thesis, rf-APGDs can be readily used for a wide-range of applications including biological decontaminations, nanostructure fabrication and portable gas analyzers.

付記する学位プログラム名: 京都大学卓越大学院プログラム「先端光・電子デバイス創成学」 / 京都大学 / 新制・課程博士 / 博士(工学) / 甲第24623号 / 工博第5129号 / 新制||工||1980(附属図書館) / 京都大学大学院工学研究科電子工学専攻 / (主査)教授 木本 恒暢, 教授 川上 養一, 准教授 浅野 卓 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

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The discovery of the ferroelectric orthorhombic phase in doped hafnia films has sparked immense research efforts. Presently, a major obstacle for hafnia's use in high-endurance memory applications like nonvolatile random-access memories is its unstable ferroelectric response during field cycling. Different mechanisms are proposed to explain this instability including field-induced phase change, electron trapping, and oxygen vacancy diffusion. However, none of these is able to fully explain the complete behavior and interdependencies of these phenomena. Up to now, no complete root cause for fatigue, wake-up, and imprint effects is presented. In this study, the first evidence for the presence of singly and doubly positively charged oxygen vacancies in hafnia–zirconia films using thermally stimulated currents and impedance spectroscopy is presented. Moreover, it is shown that interaction of these defects with electrons at the interfaces to the electrodes may cause the observed instability of the ferroelectric performance.

Ce travail étudie le rôle de la densité de trous à l’équilibre sur la dynamique des charges et de la norme de l’aimantation de (Ga,Mn)As pour des densités de manganèse et d’impuretés fixées indépendamment. Des expériences « pompe-sonde » mettent en relation les dynamiques de réflectivité et d’angle de rotation Kerr. Deux relaxations sont mises en évidence. La première traduit un échauffement variable du gaz de trous entre 1ps et 100ps. La seconde traduit une diffusion-recombinaison des charges entre 100ps et 1500ps et évolue en fonction du rapport entre extension spatiale d’états d’impuretés, piégeant les électrons photo générés, et vitesse de Fermi. Pour compléter l’approche, une étude numérique de l’état fondamental des échantillons par la théorie de la fonctionnelle de la densité relie aimantation, température et densité de trous. Elle interprète la dynamique de la norme de l’aimantation à partir d’un diagramme de phase statique correspondant aux données publiées pour (Ga,Mn)As, qui est fonction de la température et de la densité de trous. Cette dynamique se ramène à celle de la réflectivité. Ceci permet de préciser les contributions de la norme et de l’orientation de l’aimantation dans le signal dynamique de rotation Kerr. / The effects of the background hole density on the charge and magnitude of the magnetization dynamics in (Ga,Mn)As grown with independently fixed manganese and impurity densities. A pump and probe experiment monitored simultaneously the reflectivity and Kerr angle dynamics. Two relaxation steps are highlighted. First the cooling down of the charge clouds between 1ps and 100ps and second the carrier’s diffusion-recombination between 100ps and 1.500 ns. The latter depends on the ratio between the spatial extent of impurity states, which trap the photo electrons, and the Fermi velocity. To complete these experimental results, a numerical study of the ground state of the samples, using a density functional theory, relates the magnitude of the magnetization, the temperature of the carriers and the density of holes. Phase diagram are computed, and compared to already published results. We show that the magnitude of the magnetization dynamics can be fully determined from the reflectivity measurements. We conclude that it is possible to distinguish the dynamics of the magnetization magnitude and direction using the Kerr angle dynamical signal.