Rare earth praseodymium and cerium oxides have attracted intense research interest in the last few decades, due to their intriguing chemical and physical characteristics. An understanding of the correlation between structure and properties, in particular the surface chemistry, is urgently required for their application in microelectronics, catalysis, optics and other fields. Such an understanding is, however, hampered by the complexity of rare earth oxide materials and experimental methods for their characterisation. Here, we report recent progress in studying high-quality, single crystalline, praseodymium and cerium oxide films as well as ternary alloys grown on Si(111) substrates. Using these well-defined systems and based on a systematic multi-technique surface science approach, the corresponding physical and chemical properties, such as the surface structure, the surface morphology, the bulk-surface interaction and the oxygen storage/release capability, are explored in detail. We show that specifically the crystalline structure and the oxygen stoichiometry of the oxide thin films can be well controlled by the film preparation method. This work leads to a comprehensive understanding of the properties of rare earth oxides and highlights the applications of these versatile materials. Furthermore, methanol adsorption studies are performed on binary and ternary rare earth oxide thin films, demonstrating the feasibility of employing such systems for model catalytic studies. Specifically for ceria systems, we find considerable stability against normal environmental conditions so that they can be considered as a "materials bridge" between surface science models and real catalysts.
We present a versatile system for the preparation of oxide crystal surfaces in the ultra-high vacuum (UHV) at temperatures up to 1300 K. Thermal treatment is accomplished by direct current heating of a tantalum foil in contact with the oxide sample. The sample temperature is measured by a thermocouple at a position close to the crystal and its reading is calibrated against the surface temperature determined by a second thermocouple temporarily attached to the surface. The design of the sample holder is based on a transferable plate originally developed for a commercial UHV scanning probe microscope. The system is, however, also suitable for the use with electron spectroscopy or electron diffraction based surface analytical techniques. We present results for the high-temperature preparation of CeO(2)(111) surfaces with atomically flat terraces exhibiting perfect atomic order and cleanliness as revealed by non-contact atomic force microscopy (NC-AFM) imaging. NC-AFM imaging is, furthermore, used to demonstrate the temperature-controlled aggregation of gold atoms on the CeO(2)(111) surface and their evaporation at high temperatures.
We investigate properties of MBE grown photoconductive terahertz (THz) antennas based on the InGaAs/InAlAs/InP material system aimed for an excitation wavelength of approx. 1060 nm. Therefore, we analyze several different approaches concerning growth parameters, layer and material compositions as well as doping. The carrier dynamics are probed via transient white-light pump-probe spectroscopy as well as THz Time Domain Spectroscopy (TDS) measurements. We find that the electron capture probability is reduced for higher electron energies. By adjusting the material band gap this can be resolved and lifetimes of 1.3 ps are obtained. These short lifetimes enable the detection of THz TDS spectra with a bandwidth exceeding 4 THz
Optical pump-THz probe spectroscopy is used to investigate the exciton formation dynamics and its intensity dependence in bulk Ge. Associated with the intra-excitonic 1s-2p transition, the gradual build-up of an absorption peak around 3.1 meV (0.75 THz) signifies the delayed exciton formation after optical pump which is accelerated for higher excitation densities. Analyzing the spectral shape of this THz absorption resonance, two distinct resonances are found which are attributed to the mass-anisotropy of L valley electrons via a microscopic theory.
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