Diese Arbeit untersucht Fe-Oxid-Systeme mit Hilfe einer Kombination aus Mikroskopie (LEEM, Röntgen PEEMs), Beugung (LEED) und Spektroskopie (XPS) und berichtet über die elektronenoptische Entwicklung adaptiver Optiken und Aberrationskorrekturen für einen elektrostatischen abbildenden Energieanalysator. Experimentell untersuchten wir Magnetit und Hämatit Dünnschichten. Ihre Kristallstruktur, Stöchiometrie sowie deren Oberflächenterminierung können durch spezielle Herstellungsverfahren eingestellt werden. Unter Ausnutzung der Echtzeit-Beobachtung mit Mikroskopie, Beugung und Spektroskopie untersuchten wir (a) die Oberflächenmodifikationen von Fe3O4 und α-Fe2O3-Dünnschichten durch Fe Ablagerung; (b) die reversible Phasenumwandlung Fe3O4 ↔ α-Fe2O3 unter verschiedenen Oxidationsbedingungen; (c) die Bildung der metastabilen γ-Fe2O3-Phase und (d) die Wechselwirkung von Fe3O4 und α-Fe2O3 Oberflächen mit unterstützten Pt-Nanopartikeln. Es wurde ein Algorithmus entwickelt, um den LEEM Bildkontrast für inhomogene 2D Oberflächen zu simulieren. Abschließend wird das Design eines Energiefilter-System vorgestellt, das in ein PEEM/LEEM Mikroskop der neuen Generation eingebaut werden wird. Das System basiert auf dem gleichen Abbildungsprinzip wie der magnetische Ω-Filter, der erfolgreich im aktuellen SMART Mikroskop eingesetzt wird. Das neue Instrument zielt auf die Verbesserung der Orts- und Energieauflösung im XPEEM (5 nm und 70 meV). Die Mehrzahl der möglichen Aberrationen zweiter Ordnung wird durch die intrinsische Symmetrie selbstkompensiert. Die Wirkung der anderen Aberrationen wird durch ein geeignetes Design der Verzögerungs- und Beschleunigungsoptiken kombiniert mit einer optimierten Passenergie reduziert. Darüber hinaus kompensieren zusätzliche Hexapole die restlichen dominierenden Aberrationen, wodurch eine Orts- und Energieauflösung besser als 2 nm bzw. 75 meV erreicht wird. / This work presents the investigation of Fe-oxide systems, combining microscopy (LEEM, X-PEEM), diffraction (LEED) and spectroscopy (XPS), and the electron-optical development of adaptive optics and aberration corrections for an electrostatic imaging energy analyzer. Experimentally, we studied magnetite (Fe3O4) and hematite (α-Fe2O3) thin films. Their crystal structure, stoichiometry as well as their surface termination can be tuned by special preparation procedures. Taking advantage of real time observation with microscopy, diffraction and spectroscopy, we investigated (a) the surface modifications of Fe3O4 and α-Fe2O3 thin films by Fe deposition; (b) the reversible phase transformation Fe3O4 ↔ α-Fe2O3 under different oxidation conditions; (c) the formation of the metastable γ-Fe2O3 phase and (d) the interaction of Fe3O4 and α-Fe2O3 surfaces with supported Pt nanoparticles . An algorithm was developed to simulate the LEEM image contrast for inhomogeneous 2D surfaces. The possible application to experimental data and the limitation will be discussed. Finally, the design of an energy filtering system is presented, which will be implemented in a new generation PEEM/LEEM microscope. The system bases on the same imaging principle as the magnetic Ω-filter, successfully implemented in the actual SMART microscope. The new instrument aims for the improvement of lateral and energy resolution in X-PEEM (5 nm and 70 meV, respectively). The majority of the possible second order aberrations are self-compensated by intrinsic symmetry. The effect of the other aberrations is reduced by an adequate design for the deceleration-acceleration optics in combination with optimized pass energy. Furthermore, additional hexapole multipoles compensate for the residual dominating aberrations, yielding in the lateral resolution and energy resolution better than 2 nm and 75 meV, respectively.

In this thesis, the results pertaining to various investigations carried out on Triglycine sulphate (TGS) single crystals, polyvinylidene fluoride (PVDF) films, lithium tantalate (LT)/PVDF nanocomposites and LT thin films are presented with emphasis on the characteristics that are crucial for their use in pyroelectric sensors. TGS single crystals (size 68 x 45 x 42 mm3), which have high pyroelectric coefficients, were grown by slow cooling method using newly designed platform technique based crystal growth work stations. The problem of slow growth rate along c-direction was overcome by placing (010) oriented seeds on the platform. The grown TGS crystals were used for the fabrication of the laser energy meter and temperature sensor. One drawback of TGS is its low Curie temperature (490C). As a consequence when the operating temperature approaches the Curie temperature, the crystals start depolarizing owing to the movement of domains. As a result the linearity of the devices gets affected and restricts the use of TGS. Therefore pyroelectric materials possessing higher Curie temperatures and larger pyroelectric coefficients than that of TGS are desirable. LT in single crystalline form having Curie temperature of ≈6000C has already been in use for pyroelectric device applications. However, growing stoichiometric LT single crystal is very difficult. On the other hand PVDF polymer films (Tc≈1800C) have low pyrolectric coefficients and difficult to pole electrically. Therefore efforts were made to prepare LT/PVDF nanocrystal composites to increase the pyroelectric coefficient of PVDF and to reduce the poling field. Nanoparticles of LT were prepared using sol-gel route. Spherical nanoparticles of size 20-40nm were prepared from sol by adding oleic acid to it. These nanoparticles were characterized using XRD, TEM, DSC and Raman spectroscopy. PVDF films with large percentage of β-phase (ferroelectric phase) were fabricated from solutions prepared using dimethylsulphoxide (DMSO) solvent. PVDF films (30µm thick), embedded with 20-40nm sized nanocrystallites of LT were fabricated to utilize them for pyroelectric sensor applications. The ferroelectric and pyrolectric properties of nano composite films were studied for sensor applications point of view. As a replacement for the single crystals of LT in pyroelectric sensors, investigations were carried out on oriented LT thin films. The studies on LT thin films yielded promising results which could be exploited for pyroelectric sensor applications.

Nano-particle aerosols are one of the major types of air pollutants in the urban indoor and outdoor environments. Therefore, determination of mechanisms of formation, dispersion, evolution, and transformation of combustion aerosols near the major source of this type of air pollution - busy roads and road networks - is one of the most essential and urgent goals. This Thesis addresses this particular direction of research by filling in gaps in the existing physical understanding of aerosol behaviour and evolution. The applicability of the Gaussian plume model to combustion aerosols near busy roads is discussed and used for the numerical analysis of aerosol dispersion. New methods of determination of emission factors from the average fleet on a road and from different types of vehicles are developed. Strong and fast evolution processes in combustion aerosols near busy roads are discovered experimentally, interpreted, modelled, and statistically analysed. A new major mechanism of aerosol evolution based on the intensive thermal fragmentation of nano-particles is proposed, discussed and modelled. A comprehensive interpretation of mutual transformations of particle modes, a strong maximum of the total number concentration at an optimal distance from the road, increase of the proportion of small nano-particles far from the road is suggested. Modelling of the new mechanism is developed on the basis of the theory of turbulent diffusion, kinetic equations, and theory of stochastic evaporation/degradation processes. Several new powerful statistical methods of analysis are developed for comprehensive data analysis in the presence of strong turbulent mixing and stochastic fluctuations of environmental factors and parameters. These methods are based upon the moving average approach, multi-variate and canonical correlation analyses. As a result, an important new physical insight into the relationships/interactions between particle modes, atmospheric parameters and traffic conditions is presented. In particular, a new definition of particle modes as groups of particles with similar diameters, characterised by strong mutual correlations, is introduced. Likely sources of different particle modes near a busy road are identified and investigated. Strong anti-correlations between some of the particle modes are discovered and interpreted using the derived fragmentation theorem. The results obtained in this thesis will be important for accurate prediction of aerosol pollution levels in the outdoor and indoor environments, for the reliable determination of human exposure and impact of transport emissions on the environment on local and possibly global scales. This work will also be important for the development of reliable and scientifically-based national and international standards for nano-particle emissions.