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This thesis focuses on the investigation and characterization of the surfaces and interfaces of chalcopyrite-based Cu(In,Ga)Se₂ (CIGSe) and organo-metal mixed halide perovskites, specifically CH₃NH₃PbI(₃-ᵪ)Clᵪ thin film solar cell absorbers using various x-ray and electron spectroscopies. In particular, the impact of alkali treatments on the chemical and electronic surface and near-surface structure of CIGSe absorbers is studied. For CH₃NH₃PbI(₃-ᵪ)Clᵪ the compound formation is monitored and the peculiarities of the interface formation of CH₃NH₃PbI(₃-ᵪ)Clᵪ on compact and mesoporous TiO₂ are examined.
Laboratory and synchrotron-based photoelectron spectroscopy are used to gain a depth-dependent picture of the chemical and electronic structure in the surface and near-surface region of CIGSe absorbers, focusing on the influence of NaF and NaF/KF post-deposition treatments (PDT) when compared to alkali-free CIGSe absorbers. The alkali-free and NaF-PDT absorbers show similar chemical properties, having a Cu and Ga poor surface region compared to the nominal bulk and the same chemical environment for indium and selenium. For the NaF/KF-PDT samples a K-In-Se compound is present on top of a Cu-In-Ga-Se compound, with a nanopatterned surface that is almost devoid of Cu and Ga.
Further, for the NaF-PDT sample a near-surface electronic band gap of 1.61[+0.14/-0.51] eV is derived. In contrast, a large and more gradual change towards the surface is obtained for the NaF/KF-PDT absorber exhibiting a significant band gap widening of the surface, which is in agreement with a Cu- and Ga-devoid surface region and the formation of a K-In-Se surface compound.
To in-situ monitor the compound formation of CH₃NH₃PbI(₃-ᵪ)Clᵪ on compact TiO₂ (c-TiO₂) hard x-ray photoelectron spectroscopy is used. During in-situ annealing a drop-casted layer of precursor solution on c-TiO₂ shifts in the perovskite related core levels can be observed upon reach the “transition temperature” of 80-100°C. Further the Cl signal decrease at the onset of annealing and shows a depletion in the surface region for annealing temperatures above 50°C. In addition, the chemical and electronic structure of the interface between perovskite and mesoporous TiO₂ (mp-TiO₂) or c-TiO₂ using different perovskite layer thicknesses are studied.
Vortrag “ICESP XIV. International Conference on Electrostatic Precipitation 2016”, Wroclaw, Polen, 19.-23.09.2016
Back corona and dust resistivity are well known topics in electrostatic precipitation. Back corona results from high dust resistivity and occurs when the field strength in the dust layer surpasses a critical value E crit, which is typically found to be in the order of 15 to 30 kV/cm. Besides the resistivity ρ, the current density is the main parameter: E = i ρ < E crit. Hence, possible actions against back corona include a reduction of ρ by dust conditioning, or a reduction of i, for example by pulsed corona operation.
Much work has been devoted to study the dependence of ρ on dust composition, temperature, humidity, adsorption layers and dust layer porosity, and a variety of different set-ups for dust resistivity measurements has been proposed. Even though some authors report a dependence of ρ on current density or field strength resp., dust resistivity is mostly seen as a material property.
However, in measurements on product dusts in the upper resistivity range, we found that dusts show extremely non-ohmic properties:
Most strikingly, resistivity may vary by several orders of magnitude with time.
Also, the experimental arrangement can change the resistivity results by orders of magnitude: When resistivity is measured with the dust layer exposed to a corona discharge (imitating the situation in a real ESP), ρ depends strongly on the layer thickness. Meanwhile the same dust does not show the strong layer thickness dependence when electrodes are placed on both sides of the dust layer, and also time effects are much less prominent.
Additional findings include that dusts that have been exposed to resistivity measurements show a high level of electrostatic charging afterwards.
An interpretation of these results may be found from the theory of semiconductors and electret materials. Accordingly, highly resistive dust layers do not contain mobile electrons. Current transport occurs only after charge carriers (free electrons or holes) have been injected from the electrodes or from a gas discharge adjacent to the surface.
When the injection process is non-symmetric (e.g. with corona discharge), the current transport through the dust layer can be dominated by charge carriers of one polarity, depending on the polarity of the corona. Some of the effects observed in experiment, namely the layer thickness effect and the current density influence, can indeed be ascribed to unipolar injection and space charge limited conduction.
The time effects can mainly be ascribed to the “deep trapping” of the charge carriers, leading to a high level of immobile space charge. As overall space charge is limited, this reduces the level of mobile space charge available for current transport. The space charge also leads to a deformation of the electric field inside the dust layer, and hence influences injection via the Schottky (thermionic field emission) mechanism.
By integrating the mechanisms of charge transport in dielectrics (injection, drift, immobilization, recombination) into the OpenFOAM® simulation package, rather realistic simulations of time-dependent resistivity are possible. The simulations also are helpful to identify the mechanisms responsible for certain types of resistivity behavior.
Multidimensional visualization of preferential flow pathways using neutron and x-ray radiation
(2016)
The occurrence of preferential flow of water in soils is rather the rule than the exception particularly in heterogeneous structured soils. The quantitative prediction is difficult because of the spatial as well as temporal variability. One aim of the dissertation was to visualize the soil structure and flow patterns in mine soils using a combination of neutron radiography, neutron tomography and x-ray computed tomography experiments. Both radiation techniques were used to describe preferential pathways as a soil structure with CT and the process of preferential flow of water with NT. For the first time neutron radiation was applied on undisturbed soil cores to visualize water distributions in natural soils on three examples for heterogeneities of different origin.
In a first investigation we used neutron radiography to analyze the moisture distribution in undisturbed slab-type and cylindrical samples of mine soils containing lignitic fragments and inclined soil layers. 2D radiography sequences indicated that flow pathways are highly dependent on the shape, distribution, and internal structure of the lignitic fragments. For 3D experiments, the quantitative analysis of water contents failed due to a pronounced beam hardening effect. The tensiometer data indicated the existence of local non-equilibrium in pressure heads between fragments and matric pore regions.
The objective of the second study was to analyze and visualize the effects of initial soil structure formation at the surface of bare soils in an artificial hydrological catchment that has been left to undirected ecological succession for three years. The three-dimensional (3D) micro-morphology was described using the X-ray computed tomography (CT); two-dimensional (2D) infiltration patterns were obtained from drip infiltration experiments using time-resolved neutron radiography (NT). The analyses of CT data indicate the existence of (i) structural crusts on soil consisting of sandy to loamy sediments and (ii) depositional crusts on sandy sediments. The results of combined observations using CT and NT suggest that the initial soil surface structure alterations of young sandy sediment modify moisture patterns of infiltrating water only slightly.
The aim of the 3rd experiment was to study effect of two ‘ecological engineers’, moss vegetation and beetle larvae on pore structure and infiltration. The soil pore structure was characterized by micro-computed tomography analyses of bare soil, sparse and dense moss-vegetated samples containing a single burrow. Flow patterns of infiltration experiments were visualized using the neutron radiography technique. The results of this study suggest that moss vegetation and burrowing activity of ground beetles strongly control the initial soil development by modification of pore structure and surface water infiltration.
Resonance phenomena are ubiquitous in Nature. Resonance means that a system can accumulate large amounts of kinetic energy. In rotating flows inertial waves provide a mechanism for resonance by redistributing momentum, kinetic energy and helicity.
In order to investigate inertial waves a Taylor-Couette system was investigated which consists of a homogeneous liquid confined between two coaxial cylinders and two rigid lids. The inner cylinder is slightly conical (frustum) to break the vertical mirror symmetry. Inertial waves were excited by two different forcing configurations: the frustum in libration and the lids together with the outer cylinder in libration. Libration means that the rotation rate of the wall is modulated with a fixed amplitude and frequency of the order of the mean rotation rate. Direct numerical simulations (DNS) were conducted with a numerical solver in terrain-following coordinates.
DNS results reveal that inertial wave excitation is localised at the edges of the confinement, which is in very good agreement with recent laboratory measurements of Seelig (2014, PhD thesis, BTU Cottbus - Senftenberg). A model of the wave excitation mechanism was developed with the aid of boundary layer theory. The model suggests that a difference in the boundary layer mass flux (Ekman flux) excites the waves by driving an excess Ekman pumping velocity at the edges. The DNS results exhibit this flux difference, and the simulated kinetic energy spectra of the waves exhibit the frequency dependency predicted by the model.
However, DNS results also exhibit helical vortices at the edges which are not part of the model. Conservation properties suggest that these vortices are merely a compensating phenomenon which tends to stabilise the boundary layer flow. The details of this flow, however, appear less important for the wave excitation.
Response spectra of the kinetic energy, the dissipation rate, the helicity, and the quality factor were computed in order to assess resonance conditions. Simulated resonance peaks have a width of only 1/20th of the mean rotation rate. At these peaks, the kinetic energy was found to increase by a factor 10-50 even though viscous forces were still rather large (Ekman number of the order 1/100,000 with the length scale given by the mean radial gap width).
The flow patterns found at those resonances were investigated and found to be in very good agreement with the spatial patterns obtained by laboratory measurements and geometric ray tracing. The DNS results suggest that there are two types of resonance in rotating flows: modes and wave attractors. In contrast to a mode, a wave attractor exhibits net focusing of wave energy and occupies a finite frequency band. DNS results show that the wave attractor resonance frequency adjusts within the frequency band which suggests that wave attractor resonances complement 'classical' mode resonances and may, thus, be relevant in various applications.
MARCIE manual
(2016)
This manual gives an overview on MARCIE – Model Checking And Reachability analysis done effiCIEntly. MARCIE was originally developed as a symbolic model checker for stochastic Petri nets, building on its predecessor – IDDMC – Interval Decision Diagram based Model Checking – which has been previously developed for the qualitative analysis of bounded Place/Transition nets extended by special arcs. Over the last years the tool has been enriched to allow also quantitative analysis of extended stochastic Petri nets. We concentrate here on the user viewpoint. For a detailed introduction to the relevant formalisms, formal definitions and algorithms we refer to related literature.
Guided waves hold great potential for applications in the field of ultrasonic nondestructive testing. Examples of possible applications are the ultrasonic testing and structural health monitoring of wheelset-axles as used in trains. Depending on the particular type, these axles can be described as either thick cylindrical rods or thick walled hollow cylinders with varying thickness.
Wheelset-axles are safety relevant components that have to be inspected on a regular basis. The use of guided waves would allow a full inspection while accessing only the front faces of the axle, thus potentially speeding up the inspection procedure. In order to develop such an inspection technique, however, detailed knowledge of wave propagation through the axle is required.
Established mesh-based procedures, like the finite element method, could be used to simulate guided wave propagation in such structures. However, due to the size of the axle itself and the comparatively fine mesh that is dictated by the wavelengths usually applied in ultrasonic testing, these mesh-based procedures would be very expensive in terms of computation times. The multimodal approach seems to be a very promising alternative that can be expected to provide results significantly faster.
The multimodal method uses the guided wave modes of a corresponding waveguide with a constant cross-section as basis in which the local sound field at any given position in a waveguide with varying thickness can be expressed. Thereby the numerical effort is reduced to solving the one dimensional differential equations that govern the evolution of the coefficients in the mode spectrum along the waveguide. Once the sound field has been calculated, a time dependence can easily be included, which allows the simulation of pulse propagation through the waveguide.
In this thesis, the multimodal approach, as described for the calculation of Lamb-waves in plates with non-constant thickness, is extended to other types of elastic waveguides such as cylindrical rods and thick walled hollow cylinders. For the sake of simplicity, investigations are restricted to axially symmetric wave modes. The results obtained with the multimodal approach are validated against FEM-simulations. It is shown that the multimodal method potentially holds a great advantage in terms of computation time over commercially available software based on the finite element method. Finally, the multimodal method is evaluated with respect to possible future applications on wheelset-axles.
Stochastic modelling of biochemical reaction networks is getting more and more popular. Throughout the past decades typical biological models increased in their size and complexity, because of advances in systems and molecular biology, in particular through the high-throughput omic technologies. Here biochemical networks of different levels of detail are modelled, starting with simple chemical reactions and signal transduction networks, up to individual cells and entire organisms. This increases the demand for efficient analysis methods.
A Petri net is a mathematical modelling language for the description of concurrent behaviour of distributed systems. Its advantage is the ease of scalability of the models, which relates to the network’s state space, as well as the structure of the network itself.
In this work, we recall several stochastic simulation algorithms, e.g., exact as well as approximate methods. Furthermore, we introduce an approach to improve the efficiency of stochastic simulation for large and dense networks by a new approximate stochastic simulation algorithm called discrete-time leap method. We depict the wide range of simulative analyses of complex stochastic systems ranging from trace generation to the computation of transient solutions and steady state distributions. We set forth advanced analysis of stochastic models by means of simulative model checking. For the use of simulative model checking, we integrate the continuous stochastic (reward) logic (CS(R)L) and the probabilistic linear-time temporal logic with constraints (PLTLc). Simulative model checking has some limitations compared to the numerical methods, e.g., in principle it is possible to consider nested probabilistic formulas in CS(R)L, but not practical, since the calculation is not feasible in a reasonable period of time. In addition to the transient analysis, the steady state analysis is often of interest; therefore we have implemented two on-the-fly steady state detection methods. The first one is based on a “sample batch means” algorithm and is used in the linear-time temporal logic. The second approximates the steady state distribution and checks for convergence. We apply the aforementioned techniques to several case studies from systems biology and technical systems.
The main contributions of this thesis to scientific knowledge are the development of the discrete-time leap method for the simulation of stochastic models, the approximations of transient solutions and steady state distributions by use of stochastic simulation for stochastic models and Markov reward models, the development of an infinite time horizon model checking algorithm exploiting the steady state property for PLTLc and CSL, and the first simulative model checking algorithm for CSRL incorporating state and impulse rewards. All presented algorithms and methods are implemented in the advanced analysis tool MARCIE.
Nanotechnologies allow for the production of completely new materials in a wide range of industries and technical fields and are also recognised as one of the most important technological sectors for the future. The growing nanotechnological industry is rapidly generating new forms of materials; however, little is known about the behaviour of these substances, in particular their particle form and their impact on different ecological systems and the life within them. Concerns have been raised about the safety and regulation of nanomaterials, following a number of studies that indicated that some nanomaterials are able to cause adverse effects on living objects. This data, as well as increasing production volumes and commercialisation, the capability of crossing biological barriers and the increased physico-chemical activities of nanoparticles, when compared to their bulk counterparts, have triggered concern (Baró et al., 2001; Kear et al., 2012) about their impacts on health and safety.
In Germany, nanoparticles, nanotechnological products, their production processes and their disposal are generally subject to the prevailing law of the German legal system, especially with respect to the authorization of equipment, permissions regarding chemicals and other product groups, and the protection of employees and the environment. With regard to nanotechnologies, however, the question arises as to whether the present legal regulations are adequate, and/or whether regulative gaps occur because of specific new products, materials or process characteristics. Accordingly, based on the analysis of the relevant state-of-the-art technology and science, and an evaluation of existing, as well as projectable, future national legislation on this matter, this work aims to identify regulative gaps in the relevant standardisation procedures and to point out possible adjustments.
Although nanomaterials are covered by the general scope of many of the existing legislative frameworks, it is often unclear if current regulation is actually applicable for specific questions of nanomaterials and their diverse applications. In particular, there is a lack of sufficient knowledge of the risks, which could lead to imbalanced legal protection against any threats that may arise. However, it is recognised that adjustments are needed, and legal amendments have been repeatedly proposed by expert committees, policymakers, industry members and non-governmental organisations (European Parliament, 2009). Nonetheless, very few revisions have been made to date, so the existing regulations are not considered adequate to deal with all kinds of nanomaterials in both the short and long term. Current legislation needs to be adapted immediately to reflect the challenges posed by current nanomaterials and their applications.
A front-tracking algorithm for large-eddy simulation (LES) is developed to untangle the numerical and physical contributions to entrainment in stratocumulus-topped boundary layers. The front-tracking algorithm is based on the level set method. Instead of resolving the cloud-top inversion, it is represented as a discontinuous interface separating the boundary layer from the free atmosphere. The location of the interface is represented as an isosurface of an evolving marker function the evolution of which is governed by an additional transport equation. The algorithm has been implemented in an existing LES code based on the anelastic approximation of the Navier-Stokes equations.
The original LES algorithm is verified against direct-numerical simulation (DNS) data of an idealized two-dimensional cloud-top mixing layer. For this, the subgrid-scale model of the LES code was replaced by a constant molecular viscosity in order to focus on numerical errors only. A grid convergence study confirmed the anticipated global second-order rate of convergence and the convergence to the DNS solution. The slower convergence of the LES code as compared to the higher-order DNS yielded leading-order errors in the mixing layer growth at the coarsest resolutions, which were finer still than typical LES resolutions.
The front-tracking algorithm is verified by LESs of two different convective atmospheric boundary layers: the smoke cloud, a solely radiatively driven boundary layer, and a stratocumulus-topped boundary layer based on data from the DYCOMS II field study. Specifying zero entrainment, it was shown that entrainment in LES can be controlled effectively by the front-tracking algorithm. The algorithm drastically reduces entrainment errors and reduces dependencies of the solution to numerical parameters such as the choice of flux-limiters and grid resolution.
In contrast to traditional data applications, many real-world scenarios nowadays depend on managing and querying huge volumes of uncertain and incomplete data. This new type of applications emerge, for example, when we integrate data from various sources, analyse social/biological/chemical networks or conduct privacy-preserving data mining.
A very promising concept addressing this new kind of probabilistic data applications has been proposed in the form of probabilistic databases. Here, a tuple only belongs to its table or query answer with a specific likelihood. That probability expresses the uncertainty about the given data or the confidence in the answer. The most challenging task for probabilistic databases is query evaluation. In fact, there are even simple relational queries for which determining the occurrence probability of a single answer tuple is hard for #P.
Lineage formulas constitute the central concept under investigation in this work. In short, the mechanism behind lineage formulas facilitates the representation and evaluation of events of the probability space, which is defined by a probabilistic database. On the basis of lineage formulas, we devise a framework that is designed as a combination of a relational database layer and an additional probabilistic query engine.
In particular, the following three aspects are studied:
(i) an efficient construction of lineage formulas,
(ii) an orthogonal combination of lineage optimization techniques, which are performed within the relational database layer and the probabilistic query engine, and
(iii) effective and compact data structures to represent lineage formulas within a probabilistic query engine.
The developed framework provides a novel lineage construction method that is able to construct nested lineage formulas, to avoid large tuple sets within the relational database layer tuples, and to provide full relational algebra support. In addition, the proposed system completely resolves the conflict between the contradicting query plans optimized for the relational database layer and the probabilistic query engine.