Adsorbat-modifiziertes Wachstum ultradünner Seltenerdoxid-Filme auf Silizium und komplementäre Studien von Ceroxid auf Ruthenium

Abstract

Rare-earth oxides (REOx) are extensively investigated due to their extraordinary physical and chemical properties, which essentially arise from the unfilled 4f electron shell, in order to reveal the nature of these exceptional properties and ultimately to utilize them for multiple technological applications. To maintain the exponential increase in integration density in CMOS technology, which is also known as Moore s law, there is a strong desire for ultrathin, well-ordered, epitaxial REOx layers with a precisely engineered interface, which is essential for reliable, ultrahigh-performance devices. So far this has been considerably impeded by RE-promoted silicon oxidation, leading to amorphous silicon oxide and RE silicon formation. By using complementary synchrotron radiation methods such as X-ray standing waves (XSW), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD), structural and spectroscopic information are inferred simultaneously from ultrathin ceria and lanthana films grown on chlorine, silver and gallium passivated silicon(111). In general, it is revealed that the chemical and structural composition of the interface and the crystallinity of ultrathin REOx layers on silicon can be precisely controlled by adsorbate-mediated growth. This might represent a crucial step towards a perfectly engineered interface, eventually allowing for the integration of REOx as high-k gate oxides in microelectronics. In catalysis inverse model catalysts are studied with the aim of getting an in-depth understanding of the basic principles of catalysis. These model systems are employed to study, e. g., the nature of active sites and the reaction pathways in complex catalytic converters. However, a lot remains unknown about the chemical activity and selectivity as a function of the growth mechanism, structure and morphology of these model systems. The powerful spectroscopic photoemission and low-energy electron microscope, which is able to reveal the surface structure and chemical composition at nanometer resolution, is used to shed light on the growth, morphology and oxidation state of the inverse model system ceria on ruthenium(0001) up to very high growth temperatures of 1000°C. It is revealed that ceria on ruthemium(0001) forms a commensurate phase. Specifically, it is shown that the ceria island size and nucleation density can be adjusted by appropriate growth conditions, potentially giving the ability to tailor the reactivity of the catalyst through precise structural control.