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The layer-by-layer assembly (LBL) of polyelectrolytes has been extensively studied for the preparation of ultrathin films due to the versatility of the build-up process. The control of the permeability of these layers is particularly important as there are potential drug delivery applications. Multilayered polyelectrolyte microcapsules are also of great interest due to their possible use as microcontainers. This work will present two methods that can be used as employable drug delivery systems, both of which can encapsulate an active molecule and tune the release properties of the active species. Poly-(N-isopropyl acrylamide), (PNIPAM) is known to be a thermo-sensitive polymer that has a Lower Critical Solution Temperature (LCST) around 32oC; above this temperature PNIPAM is insoluble in water and collapses. It is also known that with the addition of salt, the LCST decreases. This work shows Differential Scanning Calorimetry (DSC) and Confocal Laser Scanning Microscopy (CLSM) evidence that the LCST of the PNIPAM can be tuned with salt type and concentration. Microcapsules were used to encapsulate this thermo-sensitive polymer, resulting in a reversible and tunable stimuli- responsive system. The encapsulation of the PNIPAM inside of the capsule was proven with Raman spectroscopy, DSC (bulk LCST measurements), AFM (thickness change), SEM (morphology change) and CLSM (in situ LCST measurement inside of the capsules). The exploitation of the capsules as a microcontainer is advantageous not only because of the protection the capsules give to the active molecules, but also because it facilitates easier transport. The second system investigated demonstrates the ability to reduce the permeability of polyelectrolyte multilayer films by the addition of charged wax particles. The incorporation of this hydrophobic coating leads to a reduced water sensitivity particularly after heating, which melts the wax, forming a barrier layer. This conclusion was proven with Neutron Reflectivity by showing the decreased presence of D2O in planar polyelectrolyte films after annealing creating a barrier layer. The permeability of capsules could also be decreased by the addition of a wax layer. This was proved by the increase in recovery time measured by Florescence Recovery After Photobleaching, (FRAP) measurements. In general two advanced methods, potentially suitable for drug delivery systems, have been proposed. In both cases, if biocompatible elements are used to fabricate the capsule wall, these systems provide a stable method of encapsulating active molecules. Stable encapsulation coupled with the ability to tune the wall thickness gives the ability to control the release profile of the molecule of interest.
The correction of software failures tends to be very cost-intensive because their debugging is an often time-consuming development activity. During this activity, developers largely attempt to understand what causes failures: Starting with a test case that reproduces the observable failure they have to follow failure causes on the infection chain back to the root cause (defect). This idealized procedure requires deep knowledge of the system and its behavior because failures and defects can be far apart from each other. Unfortunately, common debugging tools are inadequate for systematically investigating such infection chains in detail. Thus, developers have to rely primarily on their intuition and the localization of failure causes is not time-efficient. To prevent debugging by disorganized trial and error, experienced developers apply the scientific method and its systematic hypothesis-testing. However, even when using the scientific method, the search for failure causes can still be a laborious task. First, lacking expertise about the system makes it hard to understand incorrect behavior and to create reasonable hypotheses. Second, contemporary debugging approaches provide no or only partial support for the scientific method. In this dissertation, we present test-driven fault navigation as a debugging guide for localizing reproducible failures with the scientific method. Based on the analysis of passing and failing test cases, we reveal anomalies and integrate them into a breadth-first search that leads developers to defects. This systematic search consists of four specific navigation techniques that together support the creation, evaluation, and refinement of failure cause hypotheses for the scientific method. First, structure navigation localizes suspicious system parts and restricts the initial search space. Second, team navigation recommends experienced developers for helping with failures. Third, behavior navigation allows developers to follow emphasized infection chains back to root causes. Fourth, state navigation identifies corrupted state and reveals parts of the infection chain automatically. We implement test-driven fault navigation in our Path Tools framework for the Squeak/Smalltalk development environment and limit its computation cost with the help of our incremental dynamic analysis. This lightweight dynamic analysis ensures an immediate debugging experience with our tools by splitting the run-time overhead over multiple test runs depending on developers’ needs. Hence, our test-driven fault navigation in combination with our incremental dynamic analysis answers important questions in a short time: where to start debugging, who understands failure causes best, what happened before failures, and which state properties are infected.
Pronoun resolution normally takes place without conscious effort or awareness, yet the processes behind it are far from straightforward. A large number of cues and constraints have previously been recognised as playing a role in the identification and integration of potential antecedents, yet there is considerable debate over how these operate within the resolution process. The aim of this thesis is to investigate how the parser handles multiple antecedents in order to understand more about how certain information sources play a role during pronoun resolution. I consider how both structural information and information provided by the prior discourse is used during online processing. This is investigated through several eye tracking during reading experiments that are complemented by a number of offline questionnaire experiments. I begin by considering how condition B of the Binding Theory (Chomsky 1981; 1986) has been captured in pronoun processing models; some researchers have claimed that processing is faithful to syntactic constraints from the beginning of the search (e.g. Nicol and Swinney 1989), while others have claimed that potential antecedents which are ruled out on structural grounds nonetheless affect processing, because the parser must also pay attention to a potential antecedent’s features (e.g. Badecker and Straub 2002). My experimental findings demonstrate that the parser is sensitive to the subtle changes in syntactic configuration which either allow or disallow pronoun reference to a local antecedent, and indicate that the parser is normally faithful to condition B at all stages of processing. Secondly, I test the Primitives of Binding hypothesis proposed by Koornneef (2008) based on work by Reuland (2001), which is a modular approach to pronoun resolution in which variable binding (a semantic relationship between pronoun and antecedent) takes place before coreference. I demonstrate that a variable-binding (VB) antecedent is not systematically considered earlier than a coreference (CR) antecedent online. I then go on to explore whether these findings could be attributed to the linear order of the antecedents, and uncover a robust recency preference both online and offline. I consider what role the factor of recency plays in pronoun resolution and how it can be reconciled with the first-mention advantage (Gernsbacher and Hargreaves 1988; Arnold 2001; Arnold et al., 2007). Finally, I investigate how aspects of the prior discourse affect pronoun resolution. Prior discourse status clearly had an effect on pronoun resolution, but an antecedent’s appearance in the previous context was not always facilitative; I propose that this is due to the number of topic switches that a reader must make, leading to a lack of discourse coherence which has a detrimental effect on pronoun resolution. The sensitivity of the parser to structural cues does not entail that cue types can be easily separated into distinct sequential stages, and I therefore propose that the parser is structurally sensitive but not modular. Aspects of pronoun resolution can be captured within a parallel constraints model of pronoun resolution, however, such a model should be sensitive to the activation of potential antecedents based on discourse factors, and structural cues should be strongly weighted.
I perform and analyse the first ever calculations of rotating stellar iron core collapse in {3+1} general relativity that start out with presupernova models from stellar evolutionary calculations and include a microphysical finite-temperature nuclear equation of state, an approximate scheme for electron capture during collapse and neutrino pressure effects. Based on the results of these calculations, I obtain the to-date most realistic estimates for the gravitational wave signal from collapse, bounce and the early postbounce phase of core collapse supernovae. I supplement my {3+1} GR hydrodynamic simulations with 2D Newtonian neutrino radiation-hydrodynamic supernova calculations focussing on (1) the late postbounce gravitational wave emission owing to convective overturn, anisotropic neutrino emission and protoneutron star pulsations, and (2) on the gravitational wave signature of accretion-induced collapse of white dwarfs to neutron stars.
The sharply rising level of atmospheric carbon dioxide resulting from anthropogenic emissions is one of the greatest environmental concerns facing our civilization today. Metal-organic frameworks (MOFs) are a new class of materials that constructed by metal-containing nodes bonded to organic bridging ligands. MOFs could serve as an ideal platform for the development of next generation CO2 capture materials owing to their large capacity for the adsorption of gases and their structural and chemical tunability. The ability to rationally select the framework components is expected to allow the affinity of the internal pore surface toward CO2 to be precisely controlled, facilitating materials properties that are optimized for the specific type of CO2 capture to be performed (post-combustion capture, precombustion capture, or oxy-fuel combustion) and potentially even for the specific power plant in which the capture system is to be installed. For this reason, significant effort has been made in recent years in improving the gas separation performance of MOFs and some studies evaluating the prospects of deploying these materials in real-world CO2 capture systems have begun to emerge. We have developed six new MOFs, denoted as IFPs (IFP-5, -6, -7, -8, -9, -10, IFP = Imidazolate Framework Potsdam) and two hydrogen-bonded molecular building block (MBB, named as 1 and 2 for Zn and Co based, respectively) have been synthesized, characterized and applied for gas storage. The structure of IFP possesses 1D hexagonal channels. Metal centre and the substituent groups of C2 position of the linker protrude into the open channels and determine their accessible diameter. Interestingly, the channel diameters (range : 0.3 to 5.2 Å) for IFP structures are tuned by the metal centre (Zn, Co and Cd) and substituent of C2 position of the imidazolate linker. Moreover hydrogen bonded MBB of 1 and 2 is formed an in situ functionalization of a ligand under solvothermal condition. Two different types of channels are observed for 1 and 2. Materials contain solvent accessible void space. Solvent could be easily removed by under high vacuum. The porous framework has maintained the crystalline integrity even without solvent molecules. N2, H2, CO2 and CH4 gas sorption isotherms were performed. Gas uptake capacities are comparable with other frameworks. Gas uptake capacity is reduced when the channel diameter is narrow. For example, the channel diameter of IFP-5 (channel diameter: 3.8 Å) is slightly lower than that of IFP-1 (channel diameter: 4.2 Å); hence, the gas uptake capacity and Brunauer-Emmett-Teller (BET) surface area are slightly lower than IFP-1. The selectivity does not depend only on the size of the gas components (kinetic diameter: CO2 3.3 Å, N2 3.6 Å and CH4 3.8 ) but also on the polarizability of the surface and of the gas components. IFP-5 and-6 have the potential applications for the separation of CO2 and CH4 from N2-containing gas mixtures and CO2 and CH4 containing gas mixtures. Gas sorption isotherms of IFP-7, -8, -9, -10 exhibited hysteretic behavior due to flexible alkoxy (e.g., methoxy and ethoxy) substituents. Such phenomenon is a kind of gate effects which is rarely observed in microporous MOFs. IFP-7 (Zn-centred) has a flexible methoxy substituent. This is the first example where a flexible methoxy substituent shows the gate opening behavior in a MOF. Presence of methoxy functional group at the hexagonal channels, IFP-7 acted as molecular gate for N2 gas. Due to polar methoxy group and channel walls, wide hysteretic isotherm was observed during gas uptake. The N2 The estimated BET surface area for 1 is 471 m2 g-1 and the Langmuir surface area is 570 m2 g-1. However, such surface area is slightly higher than azolate-based hydrogen-bonded supramolecular assemblies and also comparable and higher than some hydrogen-bonded porous organic molecules.
This study investigated the warm-temperate to tropical shallow-water Miocene carbonates of the Perfugas basin (Anglona area), northern Sardinia, Italy (Central Mediterranean). The aim of this study was to identify and document the existence and significance of early diagenesis in this carbonate system, especially the diagenetic history, which reflects the diagenetic potential in terms of skeletal mineralogy. The motivation behind the present study was to investigate the role that early cementation has over facies stabilization linked to differences in biotic associations in shallow-water settings. Principal to this was to unravel the amount, kind and distribution of early cements in this type of carbonates, in order to complement previous studies, and hence acquire a more global perspective on non-tropical carbonate settings. The shallow-buried Sedini Limestone Unit was investigated for variations on early diagenetic features, as well as for the type of biotic association, and oxygen and carbon stable isotope stratigraphy. Results showed, that particularly at the Perfugas basin (< 15 km2), which evolves in time from a ramp into a steep-flanked platform, shallow-water facies are characterized by a “transitional” type of biotic association. The biotic assemblages change gradually over time from a heterozoan-rich into a photozoan-rich depositional system. This transition implies a change in the depositional environmental control factors such as temperature. It is considered that sedimentation took place under warm-temperate waters, which shifted to more warmer or tropical waters through time. Moreover, it was noticed that along with these changes, marine early syn-depositional cements (high-Mg calcite), with particular fabrics (e.g. fibrous), gradually contributed to the early lithification of rocks, favoring a steepening of the platform relief. The major controls for the shift of the depositional geometry was triggered by the change of the type of biotic associations (carbonate factory), related with the shift towards warmer conditions, and the development of early marine cementation. The identification of the amount and distribution of different cement phases, porosities and early diagenetic features, within facies and stratigraphy, showed that diagenesis is differential along depth, and within the depositional setting. High-Mg calcite cements (micrite, fibrous and syntaxial inclusion-rich) are early syn-depositional, facies-related (shallow-water), predominant at the platform phase, and marine in origin. Low-Mg calcite cements (bladed, syntaxial inclusionpoor and blocky) are early to late post-depositional, non-facies related (shallow- to deep-water) and shallow-burial marine in origin. However, a particular difference exists when looking at the amount and distribution of low-Mg calcite bladed cements. They become richer in shallow-water facies at the platform phase, suggesting that the enrichment of bladed cementation is linked to the appearance of metastable grains (e.g. aragonite). In both depositional profiles, the development of secondary porosity is the product of fabric-selective dissolution of grains (aragonite, high-Mg calcite) and/or cements (syntaxial inclusion-rich). However, stratigraphy and stable isotopes (oxygen and carbon), indicate that the molds found at shallower facies located beneath, and close to stratigraphic boundaries, have been produced by the infiltration of meteoric-derived water, which caused recrystallization without calcite cementation. Away from these stratigraphic locations, shallow- and deep-water facies show molds, and recrystallization, as well as low-Mg calcite cementation, interpreted as occurring during burial of these sediments by marine waters. The main cement source is suggested to be aragonite. Our results indicate that the Sedini Limestone Unit was transformed in three different diagenetic environments (marine, meteoric and shallow-burial marine); however, the degree of transformation in each diagenetic environment differs in the heterozoan-dominated ramp from the photozoan-dominated platform. It is suggested that the sediments from the ramp follow a diagenetic pathway similar to their heterozoan counterparts (i.e. lack of marine cementation, and loss of primary porosity by compaction), and the sediments from the platform follow a diagenetic pathway similar to their photozoan counterparts (i.e. marine cementation occluding primary porosity). However, in this carbonate setting, cements are Mg-calcite, no meteoric cementation was produced, and secondary porosity at shallow-water facies of the platform phase is mostly open and preserved. Despite the temporal and transitional change in biotic associations, ramp and platform facies (shallow- to deep-water facies) showed an oxygen isotope record overprinted by diagenesis. Oxygen primary marine signatures were not found. It is believed that burial diagenesis (recrystallization and low-Mg calcite cementation) was the main reason. This was unexpected at the ramp, since heterozoan-rich carbonates can hold isotope values close to primary marine signals due to their low-Mg calcite original composition. Ramp and platform facies (shallow- to deep-water facies) showed a carbon isotope record that was less affected by diagenesis. However, only at deep-water facies, did the carbon record show positive values comparable with carbon primary marine signals. The positive carbon values were noticed with major frequency at the platform deep-water facies. Moreover, these values usually showed a covariant trend with the oxygen isotope record; even that the latter did not hold positive values. The main conclusion of this work is that carbonates, deposited under warm-temperate to tropical conditions, have a unique facies, diagenesis and chemostratigraphic expression, which is different from their cool-water heterozoan or warm-water photozoan counterparts, reflecting the “transitional” nature of biotic association.
The interactions between peptides and lipids are of fundamental importance in the functioning of numerous membrane-mediated biochemical processes including antimicrobial peptide action, hormone-receptor interactions, drug bioavailability across the blood-brain barrier and viral fusion processes. Alteration of peptide structure could be a cause of many diseases. Biological membranes are complex systems, therefore simplified models may be introduced in order to understand processes occurring in nature. The lipid monolayers at the air/water interface are suitable model systems to mimic biological membranes since many parameters can be easily controlled. In the present work the lipid monolayers were used as a model membrane and their interactions with two different peptides B18 and Amyloid beta (1-40) peptide were investigated. B18 is a synthetic peptide that binds to lipid membranes that leads to the membrane fusion. It was demonstrated that it adopts different structures in the aqueous solutions and in the membrane interior. It is unstructured in solutions and forms alpha-helix at the air/water interface or in the membrane bound state. The peptide has affinity to the negatively charged lipids and even can fold into beta-sheet structure in the vicinity of charged membranes at high peptide to lipid ratio. It was elucidated that in the absence of electrostatic interactions B18 does not influence on the lipid structure, whereas it provides partial liquidization of the negatively charged lipids. The understanding of mechanism of the peptide action in model system may help to develop the new type of antimicrobial peptides as well as it can shed light on the general mechanisms of peptide/membrane binding. The other studied peptide - Amyloid beta (1-40) peptide, which is the major component of amyloid plaques found in the brain of patients with Alzheimer's disease. Normally the peptide is soluble and is not toxic. During aging or as a result of the disease it aggregates and shows a pronounced neurotoxicity. The peptide aggregation involves the conformational transition from a random coil or alpha-helix to beta-sheets. Recently it was demonstrated that the membrane can play a crucial role for the peptide aggregation and even more the peptide can cause the change in the cell membranes that leads to a neuron death. In the present studies the structure of the membrane bound Amyloid beta peptide was elucidated. It was found that the peptide adopts the beta-sheet structure at the air/water interface or being adsorbed on lipid monolayers, while it can form alpha-helical structure in the presence of the negatively charged vesicles. The difference between the monolayer system and the bulk system with vesicles is the peptide to lipid ratio. The peptide adopts the helical structure at low peptide to lipid ratio and folds into beta-sheet at high ratio. Apparently, Abeta peptide accumulation in the brain is concentration driven. Increasing concentration leads to a change in the lipid to peptide ratio that induces the beta-sheet formation. The negatively charged lipids can act as seeds in the plaque formation, the peptide accumulates on the membrane and when the peptide to lipid ratio increases it the peptide forms toxic beta-sheet containing aggregates.
Transcription factors (TFs) are ubiquitous gene expression regulators and play essential roles in almost all biological processes. This Ph.D. project is primarily focused on the functional characterisation of MYB112 - a member of the R2R3-MYB TF family from the model plant Arabidopsis thaliana. This gene was selected due to its increased expression during senescence based on previous qRT-PCR expression profiling experiments of 1880 TFs in Arabidopsis leaves at three developmental stages (15 mm leaf, 30 mm leaf and 20% yellowing leaf). MYB112 promoter GUS fusion lines were generated to further investigate the expression pattern of MYB112. Employing transgenic approaches in combination with metabolomics and transcriptomics we demonstrate that MYB112 exerts a major role in regulation of plant flavonoid metabolism. We report enhanced and impaired anthocyanin accumulation in MYB112 overexpressors and MYB112-deficient mutants, respectively. Expression profiling reveals that MYB112 acts as a positive regulator of the transcription factor PAP1 leading to increased anthocyanin biosynthesis, and as a negative regulator of MYB12 and MYB111, which both control flavonol biosynthesis. We also identify MYB112 early responsive genes using a combination of several approaches. These include gene expression profiling (Affymetrix ATH1 micro-arrays and qRT-PCR) and transactivation assays in leaf mesophyll cell protoplasts. We show that MYB112 binds to an 8-bp DNA fragment containing the core sequence (A/T/G)(A/C)CC(A/T)(A/G/T)(A/C)(T/C). By electrophoretic mobility shift assay (EMSA) and chromatin immunoprecipitation coupled to qPCR (ChIP-qPCR) we demonstrate that MYB112 binds in vitro and in vivo to MYB7 and MYB32 promoters revealing them as direct downstream target genes. MYB TFs were previously reported to play an important role in controlling flavonoid biosynthesis in plants. Many factors acting upstream of the anthocyanin biosynthesis pathway show enhanced expression levels during nitrogen limitation, or elevated sucrose content. In addition to the mentioned conditions, other environmental parameters including salinity or high light stress may trigger anthocyanin accumulation. In contrast to several other MYB TFs affecting anthocyanin biosynthesis pathway genes, MYB112 expression is not controlled by nitrogen limitation, or carbon excess, but rather is stimulated by salinity and high light stress. Thus, MYB112 constitutes a previously uncharacterised regulatory factor that modifies anthocyanin accumulation under conditions of abiotic stress.
The term Linked Data refers to connected information sources comprising structured data about a wide range of topics and for a multitude of applications. In recent years, the conceptional and technical foundations of Linked Data have been formalized and refined. To this end, well-known technologies have been established, such as the Resource Description Framework (RDF) as a Linked Data model or the SPARQL Protocol and RDF Query Language (SPARQL) for retrieving this information. Whereas most research has been conducted in the area of generating and publishing Linked Data, this thesis presents novel approaches for improved management. In particular, we illustrate new methods for analyzing and processing SPARQL queries. Here, we present two algorithms suitable for identifying structural relationships between these queries. Both algorithms are applied to a large number of real-world requests to evaluate the performance of the approaches and the quality of their results. Based on this, we introduce different strategies enabling optimized access of Linked Data sources. We demonstrate how the presented approach facilitates effective utilization of SPARQL endpoints by prefetching results relevant for multiple subsequent requests. Furthermore, we contribute a set of metrics for determining technical characteristics of such knowledge bases. To this end, we devise practical heuristics and validate them through thorough analysis of real-world data sources. We discuss the findings and evaluate their impact on utilizing the endpoints. Moreover, we detail the adoption of a scalable infrastructure for improving Linked Data discovery and consumption. As we outline in an exemplary use case, this platform is eligible both for processing and provisioning the corresponding information.
Reading is a complex cognitive task based on the analyses of visual stimuli. Due to the physiology of the eye, only a small number of letters around the fixation position can be extracted with high visual acuity, while the visibility of words and letters outside this so-called foveal region quickly drops with increasing eccentricity. As a consequence, saccadic eye movements are needed to repeatedly shift the fovea to new words for visual word identification during reading. Moreover, even within a foveated word fixation positions near the word center are superior to other fixation positions for efficient word recognition (O’Regan, 1981; Brysbaert, Vitu, and Schroyens, 1996). Thus, most reading theories assume that readers aim specifically at word centers during reading (for a review see Reichle, Rayner, & Pollatsek, 2003). However, saccades’ landing positions within words during reading are in fact systematically modulated by the distance of the launch site from the word center (McConkie, Kerr, Reddix, & Zola, 1988). In general, it is largely unknown how readers identify the center of upcoming target words and there is no computational model of the sensorimotor translation of the decision for a target word into spatial word center coordinates. Here we present a series of three studies which aim at advancing the current knowledge about the computation of saccade target coordinates during saccade planning in reading. Based on a large corpus analyses, we firstly identified word skipping as a further factor beyond the launch-site distance with a likewise systematic and surprisingly large effect on within-word landing positions. Most importantly, we found that the end points of saccades after skipped word are shifted two and more letters to the left as compared to one-step saccades (i.e., from word N to word N+1) with equal launch-site distances. Then we present evidence from a single saccade experiment suggesting that the word-skipping effect results from highly automatic low-level perceptual processes, which are essentially based on the localization of blank spaces between words. Finally, in the third part, we present a Bayesian model of the computation of the word center from primary sensory measurements of inter-word spaces. We demonstrate that the model simultaneously accounts for launch-site and saccade-type contingent modulations of within-word landing positions in reading. Our results show that the spatial saccade target during reading is the result of complex estimations of the word center based on incomplete sensory information, which also leads to specific systematic deviations of saccades’ landing positions from the word center. Our results have important implications for current reading models and experimental reading research.
LCST-type synthetic thermoresponsive polymers can reversibly respond to certain stimuli in aqueous media with a massive change of their physical state. When fluorophores, that are sensitive to such changes, are incorporated into the polymeric structure, the response can be translated into a fluorescence signal. Based on this idea, this thesis presents sensing schemes which transduce the stimuli-induced variations in the solubility of polymer chains with covalently-bound fluorophores into a well-detectable fluorescence output. Benefiting from the principles of different photophysical phenomena, i.e. of fluorescence resonance energy transfer and solvatochromism, such fluorescent copolymers enabled monitoring of stimuli such as the solution temperature and ionic strength, but also of association/disassociation mechanisms with other macromolecules or of biochemical binding events through remarkable changes in their fluorescence properties. For instance, an aqueous ratiometric dual sensor for temperature and salts was developed, relying on the delicate supramolecular assembly of a thermoresponsive copolymer with a thiophene-based conjugated polyelectrolyte. Alternatively, by taking advantage of the sensitivity of solvatochromic fluorophores, an increase in solution temperature or the presence of analytes was signaled as an enhancement of the fluorescence intensity. A simultaneous use of the sensitivity of chains towards the temperature and a specific antibody allowed monitoring of more complex phenomena such as competitive binding of analytes. The use of different thermoresponsive polymers, namely poly(N-isopropylacrylamide) and poly(meth)acrylates bearing oligo(ethylene glycol) side chains, revealed that the responsive polymers differed widely in their ability to perform a particular sensing function. In order to address questions regarding the impact of the chemical structure of the host polymer on the sensing performance, the macromolecular assembly behavior below and above the phase transition temperature was evaluated by a combination of fluorescence and light scattering methods. It was found that although the temperature-triggered changes in the macroscopic absorption characteristics were similar for these polymers, properties such as the degree of hydration or the extent of interchain aggregations differed substantially. Therefore, in addition to the demonstration of strategies for fluorescence-based sensing with thermoresponsive polymers, this work highlights the role of the chemical structure of the two popular thermoresponsive polymers on the fluorescence response. The results are fundamentally important for the rational choice of polymeric materials for a specific sensing strategy.
Semiclassical asymptotics for the scattering amplitude in the presence of focal points at infinity
(2006)
We consider scattering in $\R^n$, $n\ge 2$, described by the Schr\"odinger operator $P(h)=-h^2\Delta+V$, where $V$ is a short-range potential. With the aid of Maslov theory, we give a geometrical formula for the semiclassical asymptotics as $h\to 0$ of the scattering amplitude $f(\omega_-,\omega_+;\lambda,h)$ $\omega_+\neq\omega_-$) which remains valid in the presence of focal points at infinity (caustics). Crucial for this analysis are precise estimates on the asymptotics of the classical phase trajectories and the relationship between caustics in euclidean phase space and caustics at infinity.
Today, it is well known that galaxies like the Milky Way consist not only of stars but also of gas and dust. The galactic halo, a sphere of gas that surrounds the stellar disk of a galaxy, is especially interesting. It provides a wealth of information about in and outflowing gaseous material towards and away from galaxies and their hierarchical evolution. For the Milky Way, the so-called high-velocity clouds (HVCs), fast moving neutral gas complexes in the halo that can be traced by absorption-line measurements, are believed to play a crucial role in the overall matter cycle in our Galaxy. Over the last decades, the properties of these halo structures and their connection to the local circumgalactic and intergalactic medium (CGM and IGM, respectively) have been investigated in great detail by many different groups. So far it remains unclear, however, to what extent the results of these studies can be transferred to other galaxies in the local Universe. In this thesis, we study the absorption properties of Galactic HVCs and compare the HVC absorption characteristics with those of intervening QSO absorption-line systems at low redshift. The goal of this project is to improve our understanding of the spatial extent and physical conditions of gaseous galaxy halos in the local Universe. In the first part of the thesis we use HST /STIS ultraviolet spectra of more than 40 extragalactic background sources to statistically analyze the absorption properties of the HVCs in the Galactic halo. We determine fundamental absorption line parameters including covering fractions of different weakly/intermediately/highly ionized metals with a particular focus on SiII and MgII. Due to the similarity in the ionization properties of SiII and MgII, we are able to estimate the contribution of HVC-like halo structures to the cross section of intervening strong MgII absorbers at z = 0. Our study implies that only the most massive HVCs would be regarded as strong MgII absorbers, if the Milky Way halo would be seen as a QSO absorption line system from an exterior vantage point. Combining the observed absorption-cross section of Galactic HVCs with the well-known number density of intervening strong MgII absorbers at z = 0, we conclude that the contribution of infalling gas clouds (i.e., HVC analogs) in the halos of Milky Way-type galaxies to the cross section of strong MgII absorbers is 34%. This result indicates that only about one third of the strong MgII absorption can be associated with HVC analogs around other galaxies, while the majority of the strong MgII systems possibly is related to galaxy outflows and winds. The second part of this thesis focuses on the properties of intervening metal absorbers at low redshift. The analysis of the frequency and physical conditions of intervening metal systems in QSO spectra and their relation to nearby galaxies offers new insights into the typical conditions of gaseous galaxy halos. One major aspect in our study was to regard intervening metal systems as possible HVC analogs. We perform a detailed analysis of absorption line properties and line statistics for 57 metal absorbers along 78 QSO sightlines using newly-obtained ultraviolet spectra obtained with HST /COS. We find clear evidence for bimodal distribution in the HI column density in the absorbers, a trend that we interpret as sign for two different classes of absorption systems (with HVC analogs at the high-column density end). With the help of the strong transitions of SiII λ1260, SiIII λ1206, and CIII λ977 we have set up Cloudy photoionization models to estimate the local ionization conditions, gas densities, and metallicities. We find that the intervening absorption systems studied by us have, on average, similar physical conditions as Galactic HVC absorbers, providing evidence that many of them represent HVC analogs in the vicinity of other galaxies. We therefore determine typical halo sizes for SiII, SiIII, and CIII for L = 0.01L∗ and L = 0.05L∗ galaxies. Based on the covering fractions of the different ions in the Galactic halo, we find that, for example, the typical halo size for SiIII is ∼ 160 kpc for L = 0.05L∗ galaxies. We test the plausibility of this result by searching for known galaxies close to the QSO sightlines and at similar redshifts as the absorbers. We find that more than 34% of the measured SiIII absorbers have galaxies associated with them, with the majority of the absorbers indeed being at impact parameters ρ ≤160 kpc.
Nowadays, software systems are getting more and more complex. To tackle this challenge most diverse techniques, such as design patterns, service oriented architectures (SOA), software development processes, and model-driven engineering (MDE), are used to improve productivity, while time to market and quality of the products stay stable. Multiple of these techniques are used in parallel to profit from their benefits. While the use of sophisticated software development processes is standard, today, MDE is just adopted in practice. However, research has shown that the application of MDE is not always successful. It is not fully understood when advantages of MDE can be used and to what degree MDE can also be disadvantageous for productivity. Further, when combining different techniques that aim to affect the same factor (e.g. productivity) the question arises whether these techniques really complement each other or, in contrast, compensate their effects. Due to that, there is the concrete question how MDE and other techniques, such as software development process, are interrelated. Both aspects (advantages and disadvantages for productivity as well as the interrelation to other techniques) need to be understood to identify risks relating to the productivity impact of MDE. Before studying MDE's impact on productivity, it is necessary to investigate the range of validity that can be reached for the results. This includes two questions. First, there is the question whether MDE's impact on productivity is similar for all approaches of adopting MDE in practice. Second, there is the question whether MDE's impact on productivity for an approach of using MDE in practice remains stable over time. The answers for both questions are crucial for handling risks of MDE, but also for the design of future studies on MDE success. This thesis addresses these questions with the goal to support adoption of MDE in future. To enable a differentiated discussion about MDE, the term MDE setting'' is introduced. MDE setting refers to the applied technical setting, i.e. the employed manual and automated activities, artifacts, languages, and tools. An MDE setting's possible impact on productivity is studied with a focus on changeability and the interrelation to software development processes. This is done by introducing a taxonomy of changeability concerns that might be affected by an MDE setting. Further, three MDE traits are identified and it is studied for which manifestations of these MDE traits software development processes are impacted. To enable the assessment and evaluation of an MDE setting's impacts, the Software Manufacture Model language is introduced. This is a process modeling language that allows to reason about how relations between (modeling) artifacts (e.g. models or code files) change during application of manual or automated development activities. On that basis, risk analysis techniques are provided. These techniques allow identifying changeability risks and assessing the manifestations of the MDE traits (and with it an MDE setting's impact on software development processes). To address the range of validity, MDE settings from practice and their evolution histories were capture in context of this thesis. First, this data is used to show that MDE settings cover the whole spectrum concerning their impact on changeability or interrelation to software development processes. Neither it is seldom that MDE settings are neutral for processes nor is it seldom that MDE settings have impact on processes. Similarly, the impact on changeability differs relevantly. Second, a taxonomy of evolution of MDE settings is introduced. In that context it is discussed to what extent different types of changes on an MDE setting can influence this MDE setting's impact on changeability and the interrelation to processes. The category of structural evolution, which can change these characteristics of an MDE setting, is identified. The captured MDE settings from practice are used to show that structural evolution exists and is common. In addition, some examples of structural evolution steps are collected that actually led to a change in the characteristics of the respective MDE settings. Two implications are: First, the assessed diversity of MDE settings evaluates the need for the analysis techniques that shall be presented in this thesis. Second, evolution is one explanation for the diversity of MDE settings in practice. To summarize, this thesis studies the nature and evolution of MDE settings in practice. As a result support for the adoption of MDE settings is provided in form of techniques for the identification of risks relating to productivity impacts.
User-centered design processes are the first choice when new interactive systems or services are developed to address real customer needs and provide a good user experience. Common tools for collecting user research data, conducting brainstormings, or sketching ideas are whiteboards and sticky notes. They are ubiquitously available, and no technical or domain knowledge is necessary to use them. However, traditional pen and paper tools fall short when saving the content and sharing it with others unable to be in the same location. They are also missing further digital advantages such as searching or sorting content. Although research on digital whiteboard and sticky note applications has been conducted for over 20 years, these tools are not widely adopted in company contexts. While many research prototypes exist, they have not been used for an extended period of time in a real-world context. The goal of this thesis is to investigate what the enablers and obstacles for the adoption of digital whiteboard systems are. As an instrument for different studies, we developed the Tele-Board software system for collaborative creative work. Based on interviews, observations, and findings from former research, we tried to transfer the analog way of working to the digital world. Being a software system, Tele-Board can be used with a variety of hardware and does not depend on special devices. This feature became one of the main factors for adoption on a larger scale. In this thesis, I will present three studies on the use of Tele-Board with different user groups and foci. I will use a combination of research methods (laboratory case studies and data from field research) with the overall goal of finding out when a digital whiteboard system is used and in which cases not. Not surprisingly, the system is used and accepted if a user sees a main benefit that neither analog tools nor other applications can offer. However, I found that these perceived benefits are very different for each user and usage context. If a tool provides possibilities to use in different ways and with different equipment, the chances of its adoption by a larger group increase. Tele-Board has now been in use for over 1.5 years in a global IT company in at least five countries with a constantly growing user base. Its use, advantages, and disadvantages will be described based on 42 interviews and usage statistics from server logs. Through these insights and findings from laboratory case studies, I will present a detailed analysis of digital whiteboard use in different contexts with design implications for future systems.
Passive plant actuators have fascinated many researchers in the field of botany and structural biology since at least one century. Up to date, the most investigated tissue types in plant and artificial passive actuators are fibre-reinforced composites (and multilayered assemblies thereof) where stiff, almost inextensible cellulose microfibrils direct the otherwise isotropic swelling of a matrix. In addition, Nature provides examples of actuating systems based on lignified, low-swelling, cellular solids enclosing a high-swelling cellulosic phase. This is the case of the Delosperma nakurense seed capsule, in which a specialized tissue promotes the reversible opening of the capsule upon wetting. This tissue has a diamond-shaped honeycomb microstructure characterized by high geometrical anisotropy: when the cellulosic phase swells inside this constraining structure, the tissue deforms up to four times in one principal direction while maintaining its original dimension in the other. Inspired by the example of the Delosoperma nakurense, in this thesis we analyze the role of architecture of 2D cellular solids as models for natural hygromorphs. To start off, we consider a simple fluid pressure acting in the cells and try to assess the influence of several architectural parameters onto their mechanical actuation. Since internal pressurization is a configurational type of load (that is the load direction is not fixed but it “follows” the structure as it deforms) it will result in the cellular structure acquiring a “spontaneous” shape. This shape is independent of the load but just depends on the architectural characteristics of the cells making up the structure itself. Whereas regular convex tiled cellular solids (such as hexagonal, triangular or square lattices) deform isotropically upon pressurization, we show through finite element simulations that by introducing anisotropic and non-convex, reentrant tiling large expansions can be achieved in each individual cell. The influence of geometrical anisotropy onto the expansion behaviour of a diamond shaped honeycomb is assessed by FEM calculations and a Born lattice approximation. We found that anisotropic expansions (eigenstrains) comparable to those observed in the keels tissue of the Delosoperma nakurense are possible. In particular these depend on the relative contributions of bending and stretching of the beams building up the honeycomb. Moreover, by varying the walls’ Young modulus E and internal pressure p we found that both the eigenstrains and 2D elastic moduli scale with the ratio p/E. Therefore the potential of these pressurized structures as soft actuators is outlined. This approach was extended by considering several 2D cellular solids based on two types of non-convex cells. Each honeycomb is build as a lattice made of only one non-convex cell. Compared to usual honeycombs, these lattices have kinked walls between neighbouring cells which offers a hidden length scale allowing large directed deformations. By comparing the area expansion in all lattices, we were able to show that less convex cells are prone to achieve larger area expansions, but the direction in which the material expands is variable and depends on the local cell’s connectivity. This has repercussions both at the macroscopic (lattice level) and microscopic (cells level) scales. At the macroscopic scale, these non-convex lattices can experience large anisotropic (similarly to the diamond shaped honeycomb) or perfectly isotropic principal expansions, large shearing deformations or a mixed behaviour. Moreover, lattices that at the macroscopic scale expand similarly can show quite different microscopic deformation patterns that include zig-zag motions and radical changes of the initial cell shape. Depending on the lattice architecture, the microscopic deformations of the individual cells can be equal or not, so that they can build up or mutually compensate and hence give rise to the aforementioned variety of macroscopic behaviours. Interestingly, simple geometrical arguments involving the undeformed cell shape and its local connectivity enable to predict the results of the FE simulations. Motivated by the results of the simulations, we also created experimental 3D printed models of such actuating structures. When swollen, the models undergo substantial deformation with deformation patterns qualitatively following those predicted by the simulations. This work highlights how the internal architecture of a swellable cellular solid can lead to complex shape changes which may be useful in the fields of soft robotics or morphing structures.
Cellulose is the most abundant biopolymer on earth. In this work it has been used, in various forms ranging from wood to fully processed laboratory grade microcrystalline cellulose, to synthesise a variety of metal and metal carbide nanoparticles and to establish structuring and patterning methodologies that produce highly functional nano-hybrids. To achieve this, the mechanisms governing the catalytic processes that bring about graphitised carbons in the presence of iron have been investigated. It was found that, when infusing cellulose with an aqueous iron salt solution and heating this mixture under inert atmosphere to 640 °C and above, a liquid eutectic mixture of iron and carbon with an atom ratio of approximately 1:1 forms. The eutectic droplets were monitored with in-situ TEM at the reaction temperature where they could be seen dissolving amorphous carbon and leaving behind a trail of graphitised carbon sheets and subsequently iron carbide nanoparticles. These transformations turned ordinary cellulose into a conductive and porous matrix that is well suited for catalytic applications. Despite these significant changes on the nanometre scale the shape of the matrix as a whole was retained with remarkable precision. This was exemplified by folding a sheet of cellulose paper into origami cranes and converting them via the temperature treatment in to magnetic facsimiles of those cranes. The study showed that the catalytic mechanisms derived from controlled systems and described in the literature can be transferred to synthetic concepts beyond the lab without loss of generality. Once the processes determining the transformation of cellulose into functional materials were understood, the concept could be extended to other metals and metal-combinations. Firstly, the procedure was utilised to produce different ternary iron carbides in the form of MxFeyC (M = W, Mn). None of those ternary carbides have thus far been produced in a nanoparticle form. The next part of this work encompassed combinations of iron with cobalt, nickel, palladium and copper. All of those metals were also probed alone in combination with cellulose. This produced elemental metal and metal alloy particles of low polydispersity and high stability. Both features are something that is typically not associated with high temperature syntheses and enables to connect the good size control with a scalable process. Each of the probed reactions resulted in phase pure, single crystalline, stable materials. After showing that cellulose is a good stabilising and separating agent for all the investigated types of nanoparticles, the focus of the work at hand is shifted towards probing the limits of the structuring and pattering capabilities of cellulose. Moreover possible post-processing techniques to further broaden the applicability of the materials are evaluated. This showed that, by choosing an appropriate paper, products ranging from stiff, self-sustaining monoliths to ultra-thin and very flexible cloths can be obtained after high temperature treatment. Furthermore cellulose has been demonstrated to be a very good substrate for many structuring and patterning techniques from origami folding to ink-jet printing. The thereby resulting products have been employed as electrodes, which was exemplified by electrodepositing copper onto them. Via ink-jet printing they have additionally been patterned and the resulting electrodes have also been post functionalised by electro-deposition of copper onto the graphitised (printed) parts of the samples. Lastly in a preliminary test the possibility of printing several metals simultaneously and thereby producing finely tuneable gradients from one metal to another have successfully been made. Starting from these concepts future experiments were outlined. The last chapter of this thesis concerned itself with alternative synthesis methods of the iron-carbon composite, thereby testing the robustness of the devolved reactions. By performing the synthesis with partly dissolved scrap metal and pieces of raw, dry wood, some progress for further use of the general synthesis technique were made. For example by using wood instead of processed cellulose all the established shaping techniques available for wooden objects, such as CNC milling or 3D prototyping, become accessible for the synthesis path. Also by using wood its intrinsic well defined porosity and the fact that large monoliths are obtained help expanding the prospect of using the composite. It was also demonstrated in this chapter that the resulting material can be applied for the environmentally important issue of waste water cleansing. Additionally to being made from renewable resources and by a cheap and easy one-pot synthesis, the material is recyclable, since the pollutants can be recovered by washing with ethanol. Most importantly this chapter covered experiments where the reaction was performed in a crude, home-built glass vessel, fuelled – with the help of a Fresnel lens – only by direct concentrated sunlight irradiation. This concept carries the thus far presented synthetic procedures from being common laboratory syntheses to a real world application. Based on cellulose, transition metals and simple equipment, this work enabled the easy one-pot synthesis of nano-ceramic and metal nanoparticle composites otherwise not readily accessible. Furthermore were structuring and patterning techniques and synthesis routes involving only renewable resources and environmentally benign procedures established here. Thereby it has laid the foundation for a multitude of applications and pointed towards several future projects reaching from fundamental research, to application focussed research and even and industry relevant engineering project was envisioned.
Forests are a key resource serving a multitude of functions such as providing income to forest owners, supplying industries with timber, protecting water resources, and maintaining biodiversity. Recently much attention has been given to the role of forests in the global carbon cycle and their management for increased carbon sequestration as a possible mitigation option against climate change. Furthermore, the use of harvested wood can contribute to the reduction of atmospheric carbon through (i) carbon sequestration in wood products, (ii) the substitution of non-wood products with wood products, and (iii) through the use of wood as a biofuel to replace fossil fuels. Forest resource managers are challenged by the task to balance these multiple while simultaneously meeting economic requirements and taking into consideration the demands of stakeholder groups. Additionally, risks and uncertainties with regard to uncontrollable external variables such as climate have to be considered in the decision making process. In this study a scientific stakeholder dialogue with forest-related stakeholder groups in the Federal State of Brandenburg was accomplished. The main results of this dialogue were the definition of major forest functions (carbon sequestration, groundwater recharge, biodiversity, and timber production) and priority setting among them by the stakeholders using the pair-wise comparison technique. The impact of different forest management strategies and climate change scenarios on the main functions of forest ecosystems were evaluated at the Kleinsee management unit in south-east Brandenburg. Forest management strategies were simulated over 100 years using the forest growth model 4C and a wood product model (WPM). A current climate scenario and two climate change scenarios based on global circulation models (GCMs) HadCM2 and ECHAM4 were applied. The climate change scenario positively influenced stand productivity, carbon sequestration, and income. The impact on the other forest functions was small. Furthermore, the overall utility of forest management strategies were compared under the priority settings of stakeholders by a multi-criteria analysis (MCA) method. Significant differences in priority setting and the choice of an adequate management strategy were found for the environmentalists on one side and the more economy-oriented forest managers of public and private owned forests on the other side. From an ecological perspective, a conservation strategy would be preferable under all climate scenarios, but the business as usual management would also fit the expectations under the current climate. In contrast, a forest manager in public-owned forests or a private forest owner would prefer a management strategy with an intermediate thinning intensity and a high share of pine stands to enhance income from timber production while maintaining the other forest functions. The analysis served as an example for the combined application of simulation tools and a MCA method for the evaluation of management strategies under multi-purpose and multi-user settings with changing climatic conditions. Another focus was set on quantifying the overall effect of forest management on carbon sequestration in the forest sector and the wood industry sector plus substitution effects. To achieve this objective, the carbon emission reduction potential of material and energy substitution (Smat and Sen) was estimated based on a literature review. On average, for each tonne of dry wood used in a wood product substituting a non-wood product, 0.71 fewer tonnes of fossil carbon are emitted into to the atmosphere. Based on Smat and Sen, the calculation of the carbon emission reduction through substitution was implemented in the WPM. Carbon sequestration and substitution effects of management strategies were simulated at three local scales using the WPM and the forest growth models 4C (management unit level) or EFISCEN (federal state of Brandenburg and Germany). An investigation was conducted on the influence of uncertainties in the initialisation of the WPM, Smat, and basic conditions of the wood product sector on carbon sequestration. Results showed that carbon sequestration in the wood industry sector plus substitution effects exceeded sequestration in the forest sector. In contrast to the carbon pools in the forest sector, which acted as sink or source, the substitution effects continually reduced carbon emission as long as forests are managed and timber is harvested. The main climate protection function was investigated for energy substitution which accounted for about half of the total carbon sequestration, followed by carbon storage in landfills. In Germany, the absolute annual carbon sequestration in the forest and wood industry sector plus substitution effects was 19.9 Mt C. Over 50 years the wood industry sector contributed 70% of the total carbon sequestration plus substitution effects.
Phototropic microalgae have a large potential for producing valuable substances for the feed, food, cosmetics, pigment, bioremediation, and pharmacy industries as well as for biotechnological processes. Today it is estimated that the microalgal aquaculture worldwide production is 5000 tons of dry matter per year (not taking into account processed products) making it an approximately $1.25 billion U.S. per year industry. In this work, several spectroscopic techniques were utilized for the investigation of microalgae cells. Specifically, photondensity wave spectroscopy was applied as a technique for the on-line observation of the culture. For effective evaluation of the photosynthetic growth processes, fast and non-invasive sensor systems that analyze the relevant biological and technical process parameters are preferred. Traditionally, the biomass in a photobioreactor is quantified with the help of turbidimetry measurements, which require extensive calibration. Another problem frequently encountered when using spectral analysis for investigating solutions is that samples of interest are often undiluted and highly scattering and do not adhere to Beer-Lambert's law. Due to the fluorescence properties of chlorophyll, fluorescence spectroscopy techniques including fluorescence lifetime imaging and single photon counting could be applied to provide images of the cells as well as determine the effects of excitation intensity on the fluorescence lifetime, which is an indicator of the condition of the cell. A photon density wave is a sinusoidally intensity-modulated optical wave stemming from a point-source of light, which propagates through diffuse medium and exhibits amplitude and phase variations. Light propagation though strongly scattering media can be described by the P1 approximation to the Boltzmann transport equation. Photon density wave spectroscopy enables the ability to differentiate between scattered and absorbed light, which is desired so that an independent determination of the reduced scattering and absorption coefficients can be made. The absorption coefficient is related to the pigment content in the cells, and the reduced scattering coefficient can be used to characterize physical and morphological properties of the medium and was here applied for the determination of the average cell size.
Measuring the metabolite profile of plants can be a strong phenotyping tool, but the changes of metabolite pool sizes are often difficult to interpret, not least because metabolite pool sizes may stay constant while carbon flows are altered and vice versa. Hence, measuring the carbon allocation of metabolites enables a better understanding of the metabolic phenotype. The main challenge of such measurements is the in vivo integration of a stable or radioactive label into a plant without perturbation of the system. To follow the carbon flow of a precursor metabolite, a method is developed in this work that is based on metabolite profiling of primary metabolites measured with a mass spectrometer preceded by a gas chromatograph (Wagner et al. 2003; Erban et al. 2007; Dethloff et al. submitted). This method generates stable isotope profiling data, besides conventional metabolite profiling data. In order to allow the feeding of a 13C sucrose solution into the plant, a petiole and a hypocotyl feeding assay are developed. To enable the processing of large numbers of single leaf samples, their preparation and extraction are simplified and optimised. The metabolite profiles of primary metabolites are measured, and a simple relative calculation is done to gain information on carbon allocation from 13C sucrose. This method is tested examining single leaves of one rosette in different developmental stages, both metabolically and regarding carbon allocation from 13C sucrose. It is revealed that some metabolite pool sizes and 13C pools are tightly associated to relative leaf growth, i.e. to the developmental stage of the leaf. Fumaric acid turns out to be the most interesting candidate for further studies because pool size and 13C pool diverge considerably. In addition, the analyses are also performed on plants grown in the cold, and the initial results show a different metabolite pool size pattern across single leaves of one Arabidopsis rosette, compared to the plants grown under normal temperatures. Lastly, in situ expression of REIL genes in the cold is examined using promotor-GUS plants. Initial results suggest that single leaf metabolite profiles of reil2 differ from those of the WT.