We present X-ray diffraction and Raman spectroscopy investigations of a (100)-oriented (AlxGa1–x)2O3 thin film on MgO (100) and bulk-like ceramics in dependence on their composition. The thin film grown by pulsed laser deposition has a continuous lateral composition spread allowing to determine precisely the dependence of the phonon mode properties and lattice parameters on the chemical composition. For x<0.4, we observe the single-phase b-modification. Its lattice parameters and phonon energies depend linearly on the composition. We determined the slopes of these dependencies for the individual lattice parameters and for nine Raman lines, respectively. While the lattice parameters of the ceramics follow Vegard’s rule, deviations are observed for the thin film. This deviation has only a small effect on the phonon energies, which show a reasonably good agreement between thin film and ceramics.

The optimisation of the specular reflectance of solar collectors is a key parameter to increase the global yield of concentrated solar power (CSP) plants. In this work, the influence of filtered cathodic vacuum arc deposition parameters, particularly working pressure and deposition time, on the specular and diffuse reflectance of aluminium thin films, was studied. Changes in specular reflectance, measured by ultraviolet–visible and near-infrared spectroscopy (UV-vis-NIR) spectrophotometry, were directly correlated with thin film elemental concentration depth profiles, obtained by Rutherford backscattering spectrometry (RBS), and surface and cross-sectional morphologies as measured by scanning electron microscopy (SEM) and profilometry. Finally, atomic force microscopy (AFM) provided information on the roughness and growth mechanism of the films. The two contributions to the total reflectance of the films, namely diffuse and specular reflectance, were found to be deeply influenced by deposition conditions. It was proven that working pressure and deposition time directly determine the predominant factor. Specular reflectance varied from 12 to 99.8% of the total reflectance for films grown at the same working pressure of 0.1 Pa and with different deposition times. This transformation could not be attributed to an oxidation of the films as stated by RBS, but was correlated with a progressive modification of the roughness, surface, and bulk morphology of the samples over the deposition time. Hence, the evolution in the final optical properties of the films is driven by different growth mechanisms and the resulting microstructures. In addition to the originally addressed CSP applications the potential of the developed aluminium films for other application rather than CSP, such as, for example, reference material for spectroscopic diffuse reflectance measurements, is also discussed.

High power impulse magnetron sputtering has shown a lot of promise as a way of depositing photocatalytic thin films of titanium dioxide at low temperatures, however, the films deposited are often amorphous and display uncertain photocatalytic abilities. This thesis explores the deposition and characterization of photocatalytic thin films deposited with high power impulse magnetron sputtering.  Multiple films were deposited with reactive sputtering in both the oxide and metal mode of operations at different temperatures, duty cycles and substrate biases. The crystal structure, microstructure and photocatalytic activity of the samples were then characterized in order to correlate to each other as well as the growth conditions. Crystallinities were determined via a combined use of gracing incidence x-ray diffraction and Raman spectroscopy, microstructures were explored in cross-sectional images taken using scanning electron microscopy and the photocatalytic ability was measured by quantifying the rate constant during degradation of stearic acid while under UV-illumination.  It was found that the crystal structure of the sputtered films was influenced by the deposition mode used: oxide mode depositions yielded an anatase structure while metal mode depositions resulted in rutile or mixed structures. The only crystalline films were formed with substrate heating, the application of bias was found to correlate with the formation of more rutile and the most crystalline films were deposited with a higher duty cycle.  Photocatalytic films were successfully deposited at room temperature, even though they were amorphous. Interestingly, the anatase samples were not found to be the most reactive, instead it was found that the crystal structure only displayed a weak correlation to the reactivity of the films. The findings in this work suggest that the reactivity was also heavily influenced by the surface roughness of the samples as well as their microstructures.

Ultracold neutron (UCN) projection imaging is demonstrated using a boron-coated back-illuminated CCD camera and the Los Alamos UCN source. Each neutron is recorded through the capture reactions with10B. By direct detection at least one of the byproducts α, 7Li and γ (electron recoils) derived from the neutron capture and reduction of thermal noise of the scientific CCD camera, a signal-to-noise improvement on the order of 104 over the indirect detection has been achieved. Sub-pixel position resolution of a few microns is confirmed for individual UCN events. Projection imaging of test objects shows a spatial resolution less than 100μm by an integrated UCN flux one the order of 106 cm−2. The bCCD can be used to build UCN detectors with an area on the order of 1 m2. The combination of micrometer scale spatial resolution, low readout noise of a few electrons, and large area makes bCCD suitable for quantum science of UCN.

The work in this licentiate is devoted to investigating the epitaxial growth of thin Fe layers on MgAl2O4 (001) and MgO (001) substrates using dc magnetron sputtering. The aim is to qualitatively and quantitatively determine the crystal quality of the grown Fe layers depending on their thickness, substrate material, and selected deposition parameters. The effect of the crystal quality on the magnetic and electronic transport properties is discussed. The structural characterization of the epitaxial Fe thin films is carried out by x-ray reflectometry and diffraction as well as transmission electron microscopy. X-ray scattering measurements and analysis with related models allow for a quantitative determination of layering, crystal quality, and strain profiles in the growing Fe. Magnetic properties are determined using a combination of longitudinal magneto-optical Kerr effect measurements, Kerr microscopy, and scanning electron microscopy with polarization analyser. Electronic transport properties are characterized by four-point probe measurements of the thin films. The epitaxial growth of Fe is found to be highly substrate dependent: Fe layers grown on MgAl2O4 have a significantly higher crystal quality, as compared to Fe grown on MgO. The difference in crystal quality is attributed to different strain states in Fe, which is supported by theoretical calculations of the critical thickness on both substrates. Moreover, an anomalous elastic response in Fe at the thin film limit is found. The magnetic properties of Fe are weakly reflecting the differences in crystal quality of the Fe layers. However, the difference in crystal quality affects the electronic transport properties. The results of this study on epitaxial Fe layers can provide insights into strain and defect engineering in Fe thin films, which can additionally serve as model systems for finite size effects.

Philosophiae Doctor - PhD / The depletion of fossil fuel resources such as coal and the concern of climatic change arising from the emission of greenhouse gases (GHG) and global warming [1] lead to the identification of the 'hydrogen economy' as one of the renewable energy sources and possible futuristic energy conversion solution. Sources of hydrogen as fuel such as water through electrolysis and liquid organic fuel (Hydrogen carriers) have been found as potential game-changers and received increased attention, due to its low-carbon emission.

With the progression towards lighter but larger-display self-sustainable mobile devices, device efficiency becomes increasingly important, owing to the higher power display consumption but at the same time more limitation on the size and volume of energy storage. In this thesis, selected aspects regarding to efficiency of three types of optoelectronic devices, indoor photovoltaics (IPVs), perovskite thin-film transistors (TFTs) and organic light-emitting diodes (OLEDs) have been investigated. IPVs can make off-grid devices self-sustainable by harvesting ambient light energy. Its weak irradiance necessitates high-efficiency IPVs to generate sufficient power. Our work addresses the need of knowing the limit of the device parameters for correct evaluation and understanding the efficiency loss for developing clinical tactics. We delivered a general scheme for evaluating the limiting efficiency and the corresponding device parameters of IPVs under various lights, illuminance and material bandgap. In contrast to the AM1.5G conditions, a maximum power conversion efficiency (PCE) of 51-57 % can be achieved under the optimal bandgap of 1.82-1.96 eV. We also propose using the second thickness peak of interference instead of the first as a better optimal absorber thickness after identifying the finite absorption as the major source of efficiency loss. The work provides insights for device evaluation and material design for efficient IPV devices. The novel hybrid organic-inorganic perovskites have gained enormous research interest for its various excellent optoelectronic properties such as high mobility. TFT as an alternative application to the majorly focused photovoltaics is realized in this work. There are few reports on perovskite TFTs due to wetting issues. By employing polymethacrylates with ester groups and aromatic substituents which provide polar and cation-π interactions with the Pb2+ ions, quality films could be fabricated with large crystals and high electron mobility in TFTs. We further improved the performance by resolving interfacial mixing between the perovskite and the polymer using the crosslinkable SU-8, achieving the highest mobility of 1.05 cm2 V−1 s−1. Subsequently, we cured the grain boundaries using methylamine solvent vapor annealing, suppressing the TFT subthreshold swing. The work provides a map for the improvement of perovskite TFTs. It has been revealed that molecular orientations of the emitters in OLEDs with the transition dipole moment lying in plane enhances light outcoupling efficiency. Multiple experimental techniques are needed to provide complementary orientation information and their physical origin. Here, we propose using TFT to probe the orientation of the phosphorescent emitters. Homoleptic fac-Ir(ppy)3 and heteroleptic trans-Ir(ppy)2(acac) and trans-Ir(ppy)2(tmd) were deposited on polystyrene (PS) and SiO2 substrates. Compared to the PS surface inducing isotropic orientation as the control, trans-Ir(ppy)2(acac) and trans-Ir(ppy)2(tmd) possessed decreased carrier mobilities on SiO2. With the study of initial film growth, we infer that preferred orientation induced by the polar SiO2 surface led to an increase in energetic disorder in the well-stacked trans-Ir(ppy)2(acac) and hopping distance in the amorphous trans-Ir(ppy)2(tmd). The highly symmetric fac-Ir(ppy)3 remained its isotropic orientation despite the dipolar interaction. Surprisingly, the TFT technique gives much higher sensitivity to surface-induced orientation, and thus may potentially serve as a unique electrical probe for molecular orientation.

With the progression towards lighter but larger-display self-sustainable mobile devices, device efficiency becomes increasingly important, owing to the higher power display consumption but at the same time more limitation on the size and volume of energy storage. In this thesis, selected aspects regarding to efficiency of three types of optoelectronic devices, indoor photovoltaics (IPVs), perovskite thin-film transistors (TFTs) and organic light-emitting diodes (OLEDs) have been investigated. IPVs can make off-grid devices self-sustainable by harvesting ambient light energy. Its weak irradiance necessitates high-efficiency IPVs to generate sufficient power. Our work addresses the need of knowing the limit of the device parameters for correct evaluation and understanding the efficiency loss for developing clinical tactics. We delivered a general scheme for evaluating the limiting efficiency and the corresponding device parameters of IPVs under various lights, illuminance and material bandgap. In contrast to the AM1.5G conditions, a maximum power conversion efficiency (PCE) of 51-57 % can be achieved under the optimal bandgap of 1.82-1.96 eV. We also propose using the second thickness peak of interference instead of the first as a better optimal absorber thickness after identifying the finite absorption as the major source of efficiency loss. The work provides insights for device evaluation and material design for efficient IPV devices. The novel hybrid organic-inorganic perovskites have gained enormous research interest for its various excellent optoelectronic properties such as high mobility. TFT as an alternative application to the majorly focused photovoltaics is realized in this work. There are few reports on perovskite TFTs due to wetting issues. By employing polymethacrylates with ester groups and aromatic substituents which provide polar and cation-π interactions with the Pb2+ ions, quality films could be fabricated with large crystals and high electron mobility in TFTs. We further improved the performance by resolving interfacial mixing between the perovskite and the polymer using the crosslinkable SU-8, achieving the highest mobility of 1.05 cm2 V−1 s−1. Subsequently, we cured the grain boundaries using methylamine solvent vapor annealing, suppressing the TFT subthreshold swing. The work provides a map for the improvement of perovskite TFTs. It has been revealed that molecular orientations of the emitters in OLEDs with the transition dipole moment lying in plane enhances light outcoupling efficiency. Multiple experimental techniques are needed to provide complementary orientation information and their physical origin. Here, we propose using TFT to probe the orientation of the phosphorescent emitters. Homoleptic fac-Ir(ppy)3 and heteroleptic trans-Ir(ppy)2(acac) and trans-Ir(ppy)2(tmd) were deposited on polystyrene (PS) and SiO2 substrates. Compared to the PS surface inducing isotropic orientation as the control, trans-Ir(ppy)2(acac) and trans-Ir(ppy)2(tmd) possessed decreased carrier mobilities on SiO2. With the study of initial film growth, we infer that preferred orientation induced by the polar SiO2 surface led to an increase in energetic disorder in the well-stacked trans-Ir(ppy)2(acac) and hopping distance in the amorphous trans-Ir(ppy)2(tmd). The highly symmetric fac-Ir(ppy)3 remained its isotropic orientation despite the dipolar interaction. Surprisingly, the TFT technique gives much higher sensitivity to surface-induced orientation, and thus may potentially serve as a unique electrical probe for molecular orientation.

After decades of development, optical fiber technology has reached a high degree of sophistication and maturity, and currently serves as the backbone of today''s internet. Despite its technical versatility and capability, current silica fiber technology still has a significant flaw: since silica fibers only possess very weak second order nonlinearity, it has been impossible to develop a large number of important nonlinear optical devices and instruments, such as optical parametric amplifiers (OPA) and optical parametric oscillators (OPO). In this thesis,we show how to overcome this intrinsic limitation, and introduce second order nonlinearity into silica fiber devices. / Master of Science

In this thesis the influence of deposition conditions and post-deposition annealing on the structure of ultrathin iron oxide films grown on magnesium oxide (MgO) substrates is studied. The main experimental technique used is synchrotron based x-ray diffraction (XRD) but also x-ray photoelectron spectroscopy (XPS) and low energy electron diffractions (LEED) are used to characterize the samples. Studying the dependency of film structure and thickness the stoichiometry and structure is changing with increasing film thickness. For large film thickness bulk like magnetite (Fe3O4) can be observed. With decreasing thickness the oxide phase is shifting towards a wüstite (FeO) phase. When changing the deposition rate and substrate temperature a strong influence on the Fe3O4 film structure is observed. With both decreasing deposition rates and substrate temperatures the occupancy of the tetrahedral sites is strongly decreasing while the octahedral sites remain almost unaffected. By post-deposition annealing under low oxygen atmosphere it is possible to increase the ordering of the tetrahedral sites. However, this is accompanied by significant diffusion of magnesium into the iron oxide film. During post-deposition annealing of a gamma-Fe2O3 film under high vacuum a reduction of the iron oxide is observed. Increasing the temperature, first, a reduction from gamma-Fe2O3 to Fe3O4 is observed. After further increasing the temperature a reduction from Fe3O4 to FeO is observed.