No description available.

The discovery of superconductivity in iron-based pnictides in 2008 gave rise to a high advance in the research of high-temperature superconductors. But up to now there is no generally admitted theory of the non-BCS mechanism of these superconductors. The electron and hole doped Ba122 (BaFe2As2) compounds investigated in this thesis are supposed to be suitable model systems for studying the electronic behavior in order to shed light on the superconducting mechanisms. The 3d-transiton metal doped Ba122 compounds are investigated using the X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), X-ray emission spectroscopy (XES) and X-ray magnetic circular dichroism (XMCD), while the completely hole doped K122 is observed using XPS. The experimental measurements are complemented by theoretical calculations. A further new class of superconductors is represented by the electride 12CaO*7Al2O3: Here superconductivity can be realized by electrons accommodated in the crystallographic sub-nanometer-sized cavities, while the mother compound is a wide band gap insulator. Electronic structure investigations, represented by XPS, XAS and resonant X-ray photoelectron spectroscopy (ResPES), carried out in this work, should help to illuminate this unconventional superconductivity and resolve a debate of competing models for explaining the existence of superconductivity in this compound.

No description available.

No description available.

Quasi-particles formed in lithium niobate after pulse exposure were investigated by transient absorption and photoluminescence spectroscopy as well as numerical simulations. This includes the formation process, the transport through the crystal, interim pinning on defects during the relaxation process, and the final recombination with deep centers. It was shown that the charge-transport through the crystal can be described by a hopping transport including different types of hops between regular or defective lattice sites, i.e., the transport includes a mixture of free and bound small polarons. Furthermore, the different types of hops connected with varying activation energies and their distribution are responsible for an altered temporal decay curve when changing the crystal composition or temperature. Additionally, it was shown that the hitherto accepted recombination model is insufficient to describe all transient absorption and luminescence effects in lithium niobate under certain experimental conditions, i.e., long-living absorption dynamics in the blue/UV spectral range do not follow the typical polaron dynamics and cannot be described under the assumption of charge compensation. However, similar decay characteristics between self-trapped excitons known from photoluminescence spectroscopy and the unexpected behavior of the transient absorption were found leading to a revised model. This includes, besides the known polaron relaxation and recombination branch, a significant role of self-trapped excitons and their pinning on defects (pinned STEs). Since the consideration of further absorption centers in the relaxation path after pulse exposure might result in misinterpretations of previously determined polaron absorption cross-sections and shapes, the necessity to perform a review became apparent. Therefore, a supercontinuum pump-probe experiment was designed and all measurements applied under the same experimental conditions (temperature, polarization) so that one can extract the absorption amplitudes of the single quasi-particles in a spectral range of 0.7-3.0eV. The detailed knowledge might be used to deconvolve the absorption spectra and transform them to number densities of the involved centers which enables one to obtain an easier insight into recombination and decay dynamics of small polarons and self-trapped excitons. As the hopping transport of quasi-particles and the concept of pinned STEs might be fundamental processes, a thorough understanding opens up the possibility of their exploitation in various materials. In particular, results presented herein are not only limited to lithium niobate and its applications; an extension to a wide range of further strongly polar crystals in both their microscopic processes and their use in industry can be considered.

This work is dedicated to a comprehensive experimental study on the interaction of femtosecond laser pulses with the nonlinear optical medium lithium niobate. The nonlinear optical response in the nanosecond regime was already studied extensively with a variety of techniques, whereas femtosecond pulses were mainly used in transient absorption or transient grating experiments. Naturally, the temporal resolution of these measurements depends on the pulse duration, however, dynamics during the pulse excitation were barely investigated. The motivation of this work is to widen the limits of femtosecond spectroscopy, not only to temporally resolve faster nonlinear optical processes, but further to show a sensitivity to other coupling mechanisms between the pulses and the material. Especially, the role of transient, dynamic holographic gratings is investigated with a careful determination of the pulse duration, bandwidth and frequency chirp. A basis of this work is established in the first part by studying the material response via light-induced absorption before focusing on the main topic, the pulse interaction with elementary (holographic) gratings, both self-induced and static, in the second part. By this detailed study, several features of femtosecond laser pulses, holographic gratings and the ultrafast material response can be revealed: (i) grating recording is feasible even with pulses of different frequencies, provided that their pulse duration is sufficiently short, (ii) grating based pulse coupling causes a pronounced energy transfer even in a common pump-probe setup for transient absorption measurements with (non-)degenerated frequencies, (iii) beyond expectation, oscillations in the phonon frequency range become apparent in different measurements. The presented results point towards appropriate future experiments to obtain a more consistent, microscopic model for the ultrafast response of the crystal, involving the interplay between photo-generated polarons, self-induced gratings, and phonons.

Since many years, the importance of thin layers increases for lots of technical uses. Beginning in the field of microelectronics, the use of thin layers spread increasingly to other areas. Coatings for surface refining and optimisation of the mechanical properties for material engineering, customisation of the surface chemistry in catalysts, as well influencing of the transmission and reflection characteristics of surfaces in optics are only some examples of the high scientific and economic weight of the thin layer technology. Thin magnetic layers are the basis of many known storage media ranging from the tape recorder to the hard disk up to the credit card. Nowadays, these thin layers again gain interest in the research field of nanoelectronics as ultrathin layers. So-called spinvalve-read/write heads being already installed in actual hard disks use the Tunnel Magneto Resistance effect for a significant rise in memory density synonymous capacity. Such read/writeheads consist of a magnetic layersystem. This use of the magnetic as well as the electric characteristics of the electrons is called spintronics. The iron oxide magnetite exhibits a high iron portion, is strong antiferrimagnetic and has a high Curie-temperature. Since many years, it is used as a magnetic pigment on already mentioned magnetic tapes. Literature [1, 2, 3, 4] considers ultrathin epitaxial layers of magnetite on magnesium oxide for uses in the spintronics as a most promising candidate, because it inheres a complete spin polarisation at Fermi-level. Moreover, thin magnetite layers serve in the chemical industry as a catalyst in the Haber- Bosch-procedure and to the dehydration of ethylbenzene to styrene. Being already used and considered to be of ongoing interest, ultrathin magnetite layers offer a wide range of technological applications in many modern industrial and scientific fields. Because there is, nevertheless, a variety of other iron oxide (cf. chapter 4), it is a matter to determine the special growth conditions of magnetite. These ultrathin iron oxide layers were grown reactively on the (001)-surfaces of the magnesium oxide substrate by molecular beam epitaxy. Besides, the surface is examined by the diffraction of low-energy electrons concerning its crystalline structure. X-ray photo electron spectroscopy approaching the stochiometry completes these first characterisations. Other investigations are carried out at HASYLAB / DESY in Hamburg by X-ray reflectivity and X-ray diffraction. The exact thickness of the layers, its crystal properties in bulk, as well as the thickness of the crystalline portion of the layers can be determined among other features of the system. The evaluation of XRR-and XRD-investigations is done via simulations with in chapter 5 introduced software packages. The reader finds the theoretical backgrounds to the used techniques in chapter 3. The experimental setups in Osnabr¨uck and Hamburg as well as the backgrounds to the preparation are presented in chapter 5. Because the formation of the different iron oxides is described in literature [5, 6, 7, 8] as mostly depending on annealing temperatures, the experimental results in chapter 6 are graded accordingly. The dependence on temperature, layer thickness and annealing time should be examined for the iron oxides possible on this substrate. The aim of this work is the preparation of ultrathin epitaxial iron oxide layers with thicknesses up to few nanometers. The main goal is to find the growth parameters for ultrathin crystalline magnetite layers.

Die Elektronen-Spin-Resonanz-Spektroskopie (ESR) in Verbindung mit ortsspezifischer Spinmarkierung stellt eine hervorragende Möglichkeit dar, um die Struktur und Dynamik von Proteinen aufzuklären. In dieser Dissertation wurden mit Hilfe der Hochfeld-ESR-Spektroskopie (W-Band, 95 GHz, T=160 K) für dreizehn spinmarkierte Colicin A Proben die Polarität und die Protizität der Umgebung der Spinlabelbindestelle bestimmt. Wasserzugänglichkeiten und Wasserstoffbrückenbindungen zum Spinlabel wurden mittels Puls-ESR Methoden (3-Puls-D-ESEEM und Hahn-Echozerfall) bestimmt und die Ergebnisse mit den Polaritäts- und Protizitätswerten korreliert. Raumtemperaturspektren dieser Proben im X-Band (9.5 GHz), Q-Band (34 GHz) und W-Band (95 GHz) liefern Informationen über die Spinlabelbewegung. Mit Hilfe von Molekulardynamiksimulationen (MD) der spinmarkierten kanalbildenden Domäne von Colicin A konnten die Konformationen (Rotameranalyse) und die Dynamik der Spinlabelseitenketten in den unterschiedlichen Umgebungen charakterisiert werden. Der Vergleich der experimentellen mit den aus MD-Trajektorien berechneten ESR-Spektren liefert die Beiträge der unterschiedlichen Rotamerübergänge, die für die beobachteten Spektrenformen charakteristisch sind.

Thin metallic films with magnetic properties like magnetite are an interesting material in current technological applications. In the presented work the iron oxide films are grown by molecular beam epitaxy on MgO(001) substrates at temperatures between room temperature and 600K. The film and surface structure are investigated by x-ray reflectometry (XRR), x-ray diffraction (XRD) and low energy electron diffraction (LEED). The chemical properties are investigated by x-ray photoelectron spectroscopy (XPS). Furthermore, charge transfer multiplet (CTM) calculations are performed as a means to gain additional information from photoemission spectra. It is shown that only for temperatures higher than 500K the oxide film forms a spinel structure. A previously unobserved (2x1) surface reconstruction in two orthogonal domains is found for various preparation conditions. The application of CTMs results in good quantitative and qualitative agreement to other methods for the determination of the film stoichiometry. In addition CTMs can well describe the segregation of Mg atoms into the oxide film either during film growth or during film annealing. It is found that initially Mg substitutes Fe on all possible lattice sites, only for prolonged treatment at high temperature do Mg atoms favour the octahedral lattice sites of divalent Fe.

The present work broaches the physics of light-matter interaction, chiefly using nonlinear optical spectroscopy in a newly developed framework termed as Photon Management Concept. This way, existing fragments dealing with specific properties of harmonic and upconversion nanoparticles (HNPs/UCNPs) are consolidated into a full and coherent picture with the primary goal of understanding the underlying physical processes and their impact on the application side, especially in terms of imaging techniques, via suitable experimental and numerical studies. Contemporary optical setups involving contrast-enhancing agents are frequently limited in their excitation and detection configurations owing to a specialization to a select number of markers. As a result, the bandwidth of experimental methods and specimens that may be investigated is severely restricted in a large number of state-of-the-art setups. Here, an alternative approach involving HNPs and UCNPs, respectively, is presented providing an overview from their synthesis to optical characterization and to potential fields of application. Based on their inherent flexibility based on their nonlinear optical response, especially in terms of wavelength and intensity tunability, the PMC alleviates prevalent limitations by dynamically adapting the setup to a sample instead of the preliminary culling to a reduced number of eligible specimens that must not change their optical properties significantly during investigation. The use of HNPs supersedes such concerns due to their nearly instantaneously generated, strongly anti-Stokes shifted, coherent emission capable of producing radiation throughout the visible spectral range, including infrared and ultraviolet wavelengths. This way, HNPs transcend the traditional field of imaging and introduces potential applications in optomanipulation or holographic techniques. Thorough (nonlinear) optical characterization of UCNPs and alkali niobate HNP ensembles is performed to assess the fundamental physical mechanisms interwoven with numerical studies leading to their wide-ranging applicability. Final remarks show that HNPs are ideal candidates for realization of the PMC and yet hold an even further potential beyond current prospects.