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The present work investigates the structure formation and wetting in two dimensional (2D) Langmuir monolayer phases in local thermodynamic equilibrium. A Langmuir monolayer is an isolated 2D system of surfactants at the air/water interface. It exhibits crystalline, liquid crystalline, liquid and gaseous phases differing in positional and/or orientational order. Permanent electric dipole moments of the surfactants lead to a long range repulsive interaction and to the formation of mesoscopic patterns. An interaction model is used describing the structure formation as a competition between short range attraction (bare line tension) and long range repulsion (surface potentials) on a scale Delta. Delta has the meaning of a dividing length between the short and long range interaction. In the present work the thermodynamic equilibrium conditions for the shape of two phase boundary lines (Young-Laplace equation) and three phase intersection points (Young′s condition) are derived and applied to describe experimental data: The line tension is measured by pendant droplet tensiometry. The bubble shape and size of 2D foams is calculated numerically and compared to experimental foams. Contact angles are measured by fitting numerical solutions of the Young-Laplace equation on micron scale. The scaling behaviour of the contact angle allows to measure a lower limit for Delta. Further it is discussed, whether in biological membranes wetting transitions are a way in order to control reaction kinetics. Studies performed in our group are discussed with respect to this question in the framework of the above mentioned theory. Finally the apparent violation of Gibbs′ phase rule in Langmuir monolayers (non-horizontal plateau of the surface pressure/area-isotherm, extended three phase coexistence region in one component systems) is investigated quantitatively. It has been found that the most probable explanation are impurities within the system whereas finite size effects or the influence of the long range electrostatics can not explain the order of magnitude of the effect.
This thesis discusses heat and charge transport phenomena in single-crystalline Silicon penetrated by nanometer-sized pores, known as mesoporous Silicon (pSi). Despite the extensive attention given to it as a thermoelectric material of interest, studies on microscopic thermal and electronic transport beyond its macroscopic characterizations are rarely reported. In contrast, this work reports the interplay of both.
PSi samples synthesized by electrochemical anodization display a temperature dependence of specific heat 𝐶𝑝 that deviates from the characteristic 𝑇^3 behaviour (at 𝑇<50𝐾). A thorough analysis reveals that both 3D and 2D Einstein and Debye modes contribute to this specific heat. Additional 2D Einstein modes (~3 𝑚𝑒𝑉) agree reasonably well with the boson peak of SiO2 in pSi pore walls. 2D Debye modes are proposed to account for surface acoustic modes causing a significant deviation from the well-known 𝑇^3 dependence of 𝐶𝑝 at 𝑇<50𝐾.
A novel theoretical model gives insights into the thermal conductivity of pSi in terms of porosity and phonon scattering on the nanoscale. The thermal conductivity analysis utilizes the peculiarities of the pSi phonon dispersion probed by the inelastic neutron scattering experiments. A phonon mean-free path of around 10 𝑛𝑚 extracted from the presented model is proposed to cause the reduced thermal conductivity of pSi by two orders of magnitude compared to p-doped bulk Silicon. Detailed analysis indicates that compound averaging may cause a further 10-50% reduction. The percolation threshold of 65% for thermal conductivity of pSi samples is subsequently determined by employing theoretical effective medium models.
Temperature-dependent electrical conductivity measurements reveal a thermally activated transport process. A detailed analysis of the activation energy 𝐸𝐴𝜎 in the thermally activated transport exhibits a Meyer Neldel compensation rule between different samples that originates in multi-phonon absorption upon carrier transport. Activation energies 𝐸𝐴𝑆 obtained from temperature-dependent thermopower measurements provide further evidence for multi-phonon assisted hopping between localized states as a dominant charge transport mechanism in pSi, as they systematically differ from the determined 𝐸𝐴𝜎 values.
With the implementation of intense, short pulsed light sources throughout the last years, the powerful technique of resonant inelastic X-ray scattering (RIXS) became feasible for a wide range of experiments within femtosecond dynamics in correlated materials and molecules.
In this thesis I investigate the potential to bring RIXS into the fluence regime of nonlinear X-ray-matter interactions, especially focusing on the impact of stimulated scattering on RIXS in transition metal systems in a transmission spectroscopy geometry around transition metal L-edges.
After presenting the RIXS toolbox and the capabilities of free electron laser light sources for ultrafast intense X-ray experiments, the thesis explores an experiment designed to understand the impact of stimulated scattering on diffraction and direct beam transmission spectroscopy on a CoPd multilayer system. The experiments require short X-ray pulses that can only be generated at free electron lasers (FEL). Here the pulses are not only short, but also very intense, which opens the door to nonlinear X-ray-matter interactions. In the second part of this thesis, we investigate observations in the nonlinear interaction regime, look at potential difficulties for classic spectroscopy and investigate possibilities to enhance the RIXS through stimulated scattering. Here, a study on stimulated RIXS is presented, where we investigate the light field intensity dependent CoPd demagnetization in transmission as well as scattering geometry. Thereby we show the first direct observation of stimulated RIXS as well as light field induced nonlinear effects,
namely the breakdown of scattering intensity and the increase in sample transmittance. The topic is of ongoing interest and will just increase in relevance as more free electron lasers are planned and the number of experiments at such light sources will continue to increase in the near future.
Finally we present a discussion on the accessibility of small DOS shifts in the absorption-band of transition metal complexes through stimulated resonant X-ray scattering. As these shifts occur for example in surface states this finding could expand the experimental selectivity of NEXAFS and RIXS to the detectability of surface states. We show how stimulation can indeed enhance the visibility of DOS shifts through the detection of stimulated spectral shifts and enhancements in this theoretical study. We also forecast the observation of stimulated enhancements in resonant excitation experiments at FEL sources in systems with a high density of states just below the Fermi edge and in systems with an occupied to unoccupied DOS ratio in the valence band above 1.
In der nichtlinearen Datenreihenanalyse hat sich seit etwa 10 Jahren eine Monte-Carlo-Testmethode etabliert, die Theiler-surrogatmethode, mit Hilfe derer entschieden werden kann, ob eine Datenreihe nichtlinearen Ursprungs sei. Diese Methode wird kritisiert, modifiziert und verallgemeinert. Das, was Theiler untersuchen will braucht andere Surrogatmethoden, die hier konstruiert werden. Und das, was Theiler untersucht braucht gar keine Monte-Carlo-Methoden. Mit Hilfe des in der Arbeit eingeführten Begriffs des Phasensignals werden Testmöglichkeiten dargelegt und Beziehungen zwischen den nichtlinearen Eigenschaften der Zeitreihe und deren Phasenspektrum erforscht. Das Phasensignal wird aus dem Phasenspektrum der Zeitreihe hergeleitet und registriert außerordentliche Geschehnisse im Zeitbereich sowie Phasenkopplungen im Frequenzbereich. Die gewonnenen Erkenntnisse werden auf das Problem der Polbewegung angewendet. Die Hypothese einer nichtlinearen Beziehung zwischen der atmosphärischen Erregung und der Polbewegung wird untersucht. Eine nichtlineare Behandlung wird nicht für nötig gehalten.
Die Fusion von Membranen ist ein entscheidender Prozeß bei der Entwicklung von Zellen im Körper. Beispielsweise ist sie eine der Voraussetzungen bei der Befruchtung einer Eizelle durch ein Spermium oder für das Eindringen von Viren in eine Zelle. Membranfusion ist auch notwendig für den Stofftransport in die Zelle hinein oder aus ihr heraus. Die Membranfusion ist daher auch von praktischen Interesse auf den Gebieten der Pharmazeutik und des 'Bioengineering'. Oft muss eine Membran mit der infiziertin Zelle fusionieren, um ein Medikament an sein Zeil zu bringen. Deshalb ist ein Verständnis der Membranfusion von großem Interesse für die Entwicklung von gezielten und effizienten Methoden des 'drug delivery'. Dasselbe gilt für die gezielte Zufuhr von Genen bei der Gentherapie. Obwohl die Membranfusion schon vor nahezu 200 Jahren von dem deutschen Biologen und Mediziner Johannes Müller beobachtet wurde, liegt ein vollständiges Verständnis des Fusionsprozesses von Zellen und (Modell-) Membranen auch heute noch in weiter Ferne. Allerdings hat im letzten Jahrzehnt das Interesse für dieses Forschungsgebiet stark zugenommen. Wissenschaftler der unterschiedlichsten Disziplinen arbeiten daran, die Mechanismen der Membranfusion aufzudecken. Biologen untersuchen Proteine, die die Fusion auslösen, Chemiker entwickeln Moleküle, die die Fusion erleichtern, und Physiker versuchen die Antriebsmechanismen der Membranfusion zu verstehen. Neue Mikroskopietechniken und die hohe Rechenleistung moderner Computer helfen die molekulare und die makroskopische Welt der Membranfusion in einem Bild zusammenzufügen. Für unsere Untersuchungen haben wir Modellmembranen, die aus Lipiddoppelschichten bestehen, benutzt. Diese Membranen formen sogenannte Vesikel oder Liposomen, abgeschlossene Membrane, in denen eine bestimmte Menge an Flüssigkeit enthalten ist. Indem wir Rezeptoren in die Membran einbringen, schaffen wir funkionalisierte Vesikel, die sich differenzieren, kooperieren und selektiv reagieren können. Wir benutzen positiv geladene wasserlösliche Ionen, um Wechselwirkungen zwischen den Vesikeln zu vermitteln, und lassen die Rezeptoren und die Ionen den Fusionsprozess auslösen. Die Wechselwirkungen werden unter dem Mikroskop durch spezielle Mikromechanischn Gerätz Mikromechinerien kontrolliert. Mit Hilfe einer sehr schnellen digitale Bildaufnahmetechnik ist es uns gelungen, die Fusion unserer Modellmembranen aufzunehmen und in Echtzeit zu dokumentieren mit einer Auflösung von 50 µs. Unsere Messungen können vergleichen werden mit Computersimulationen des Fusionsprozesses. Diese Simulationen untersuchen Prozesse, die zwischen 0.1 und 1 Mikrosekunde dauern. Eine Herausforderung für die Zukunft wird es sein, die Lücke zwischen den in Experimenten (50µs) und den in Simulationen zugänglichen Zeitskalen von beiden Seiten her zu schließen.
Diese Arbeit beschäftigt sich mit der Annahme, dass den Erdbeben ein selbstorganisiert kritischer Zustand der Erdkruste zugrunde liegt. Mit Hilfe einer Erweiterung bisheriger Modelle wird gezeigt, dass ein solcher Zustand nicht nur für die Grössenverteilung der Erdbeben (Gutenberg-Richter Gesetz), sondern auch für das beobachtete raumzeitliche Auftreten, z.B. für das Omori-Gesetz für Nachbebenserien, verantwortlich sein kann. Desweiteren wird die Frage nach der Vorhersagbarkeit grosser Erdbeben in solchen Modellsimulationen untersucht.
This thesis investigates the Casimir effect between plates made of normal and superconducting metals over a broad range of temperatures, as well as the Casimir-Polder interaction of an atom to such a surface. Numerical and asymptotical calculations have been the main tools in order to do so. The optical properties of the surfaces are described by dielectric functions or optical conductivities, which are reviewed for common models and have been analyzed with special weight on distributional properties and causality. The calculation of the Casimir energy between two normally conducting plates (cavity) is reviewed and previous work on the contribution to the Casimir energy due to the surface plasmons, present in all metallic cavities, has been generalized to finite temperatures for the first time. In the field of superconductivity, a new analytical continuation of the BCS conductivity to to purely imaginary frequencies has been obtained both inside and outside the extremely dirty limit of vanishing mean free path. The Casimir free energy calculated from this description was shown to coincide well with the values obtained from the two fluid model of superconductivity in certain regimes of the material parameters. The Casimir entropy in a superconducting cavity fulfills the third law of thermodynamics and features a characteristic discontinuity at the phase transition temperature. These effects were equally encountered in the Casimir-Polder interaction of an atom with a superconducting wall. The magnetic dipole coupling of an atom to a metal was shown to be highly sensible to dissipation and especially to the surface currents. This leads to a strong quenching of the magnetic Casimir-Polder energy at finite temperature. Violations of the third law of thermodynamics are encountered in special models, similar to phenomena in the Casimir-effect between two plates, that are debated controversely. None of these effects occurs in the analog electric dipole interaction. The results of this work suggest to reestablish the well-known plasma model as the low temperature limit of a superconductor as in London theory rather than use it for the description of normal metals. Superconductors offer the opportunity to control the dissipation of surface currents to a great extent. This could be used to access experimentally the low frequency optical response of metals, which is strongly connected to the thermal Casimir-effect. Here, differently from corresponding microwave experiments, energy and momentum are independent quantities. A measurement of the total Casimir-Polder interaction of atoms with superconductors seems to be in reach in today’s microchip-based atom-traps and the contribution due to magnetic coupling might be accessed by spectroscopic techniques
Thermal and quantum fluctuations of the electromagnetic near field of atoms and macroscopic bodies play a key role in quantum electrodynamics (QED), as in the Lamb shift. They lead, e.g., to atomic level shifts, dispersion interactions (Van der Waals-Casimir-Polder interactions), and state broadening (Purcell effect) because the field is subject to boundary conditions. Such effects can be observed with high precision on the mesoscopic scale which can be accessed in micro-electro-mechanical systems (MEMS) and solid-state-based magnetic microtraps for cold atoms (‘atom chips’). A quantum field theory of atoms (molecules) and photons is adapted to nonequilibrium situations. Atoms and photons are described as fully quantized while macroscopic bodies can be included in terms of classical reflection amplitudes, similar to the scattering approach of cavity QED. The formalism is applied to the study of nonequilibrium two-body potentials. We then investigate the impact of the material properties of metals on the electromagnetic surface noise, with applications to atomic trapping in atom-chip setups and quantum computing, and on the magnetic dipole contribution to the Van der Waals-Casimir-Polder potential in and out of thermal equilibrium. In both cases, the particular properties of superconductors are of high interest. Surface-mode contributions, which dominate the near-field fluctuations, are discussed in the context of the (partial) dynamic atomic dressing after a rapid change of a system parameter and in the Casimir interaction between two conducting plates, where nonequilibrium configurations can give rise to repulsion.
The molecular ability to selectively and efficiently convert sunlight into other forms of energy like heat, bond change, or charge separation is truly remarkable. The decisive steps in these transformations often happen on a femtosecond timescale and require transitions among different electronic states that violate the Born-Oppenheimer approximation (BOA). Non-BOA transitions pose challenges to both theory and experiment. From a theoretical point of view, excited state dynamics and nonadiabatic transitions both are difficult problems (see Figure 1(a)). However, the theory on non-BOA dynamics has advanced significantly over the last two decades. Full dynamical simulations for molecules of the size of nucleobases have been possible for a couple of years and allow predictions of experimental observables like photoelectron energy or ion yield. The availability of these calculations for isolated molecules has spurred new experimental efforts to develop methods that are sufficiently different from all optical techniques. For determination of transient molecular structure, femtosecond X-ray diffraction and electron diffraction have been implemented on optically excited molecules.
This Thesis was devoted to the study of the coupled system composed by El Niño/Southern Oscillation and the Annual Cycle. More precisely, the work was focused on two main problems: 1. How to separate both oscillations into an affordable model for understanding the behaviour of the whole system. 2. How to model the system in order to achieve a better understanding of the interaction, as well as to predict future states of the system. We focused our efforts in the Sea Surface Temperature equations, considering that atmospheric effects were secondary to the ocean dynamics. The results found may be summarised as follows: 1. Linear methods are not suitable for characterising the dimensionality of the sea surface temperature in the tropical Pacific Ocean. Therefore they do not help to separate the oscillations by themselves. Instead, nonlinear methods of dimensionality reduction are proven to be better in defining a lower limit for the dimensionality of the system as well as in explaining the statistical results in a more physical way [1]. In particular, Isomap, a nonlinear modification of Multidimensional Scaling methods, provides a physically appealing method of decomposing the data, as it substitutes the euclidean distances in the manifold by an approximation of the geodesic distances. We expect that this method could be successfully applied to other oscillatory extended systems and, in particular, to meteorological systems. 2. A three dimensional dynamical system could be modeled, using a backfitting algorithm, for describing the dynamics of the sea surface temperature in the tropical Pacific Ocean. We observed that, although there were few data points available, we could predict future behaviours of the coupled ENSO-Annual Cycle system with an accuracy of less than six months, although the constructed system presented several drawbacks: few data points to input in the backfitting algorithm, untrained model, lack of forcing with external data and simplification using a close system. Anyway, ensemble prediction techniques showed that the prediction skills of the three dimensional time series were as good as those found in much more complex models. This suggests that the climatological system in the tropics is mainly explained by ocean dynamics, while the atmosphere plays a secondary role in the physics of the process. Relevant predictions for short lead times can be made using a low dimensional system, despite its simplicity. The analysis of the SST data suggests that nonlinear interaction between the oscillations is small, and that noise plays a secondary role in the fundamental dynamics of the oscillations [2]. A global view of the work shows a general procedure to face modeling of climatological systems. First, we should find a suitable method of either linear or nonlinear dimensionality reduction. Then, low dimensional time series could be extracted out of the method applied. Finally, a low dimensional model could be found using a backfitting algorithm in order to predict future states of the system.