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- Institut für Geowissenschaften (20)
- Institut für Physik und Astronomie (20)
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Be Creative, Now!
(2018)
Purpose – This thesis set out to explore, describe, and evaluate the reality behind the rhetoric of freedom and control in the context of creativity. The overarching subject is concerned with the relationship between creativity, freedom, and control, considering freedom is also seen as an element of control to manage creativity.
Design/methodology/approach – In-depth qualitative data gathered from at two innovative start-ups. Two ethnographic studies were conducted. The data are based on participatory observations, interviews, and secondary sources, each of which included a three months field study and a total of 41 interviews from both organizations.
Findings – The thesis provides explanations for the practice of freedom and the control of creativity within organizations and expands the existing theory of neo-normative control. The findings indicate that organizations use complex control systems that allow a high degree of freedom that paradoxically leads to more control. Freedom is a cover of control, which in turn leads to creativity. Covert control even results in the responsibility to be creative outside working hours.
Practical implications – Organizations, which rely on creativity might use the results of this thesis. Positive workplace control of creativity provides both freedom and structure for creative work. While freedom leads to organizational members being more motivated and committing themselves more strongly to their and the organization’s goals, and a specific structure also helps to provide the requirements for creativity.
Originality/value – The thesis provides an insight into an approach to workplace control, which has mostly neglected in creativity research and proposes a modified concept of neo-normative control. It serves to provide a further understanding of freedom for creativity and to challenge the liberal claims of new control forms.
The aim of this doctoral thesis was to establish a technique for the analysis of biomolecules with infrared matrix-assisted laser dispersion (IR-MALDI) ion mobility (IM) spectrometry. The main components of the work were the characterization of the IR-MALDI process, the development and characterization of different ion mobility spectrometers, the use of IR-MALDI-IM spectrometry as a robust, standalone spectrometer and the development of a collision cross-section estimation approach for peptides based on molecular dynamics and thermodynamic reweighting.
First, the IR-MALDI source was studied with atmospheric pressure ion mobility spectrometry and shadowgraphy. It consisted of a metal capillary, at the tip of which a self-renewing droplet of analyte solution was met by an IR laser beam. A relationship between peak shape, ion desolvation, diffusion and extraction pulse delay time (pulse delay) was established. First order desolvation kinetics were observed and related to peak broadening by diffusion, both influenced by the pulse delay. The transport mechanisms in IR-MALDI were then studied by relating different laser impact positions on the droplet surface to the corresponding ion mobility spectra. Two different transport mechanisms were determined: phase explosion due to the laser pulse and electrical transport due to delayed ion extraction. The velocity of the ions stemming from the phase explosion was then measured by ion mobility and shadowgraphy at different time scales and distances from the source capillary, showing an initially very high but rapidly decaying velocity. Finally, the anatomy of the dispersion plume was observed in detail with shadowgraphy and general conclusions over the process were drawn.
Understanding the IR-MALDI process enabled the optimization of the different IM spectrometers at atmospheric and reduced pressure (AP and RP, respectively). At reduced pressure, both an AP and an RP IR-MALDI source were used. The influence of the pulsed ion extraction parameters (pulse delay, width and amplitude) on peak shape, resolution and area was systematically studied in both AP and RP IM spectrometers and discussed in the context of the IR-MALDI process. Under RP conditions, the influence of the closing field and of the pressure was also examined for both AP and RP sources. For the AP ionization RP IM spectrometer, the influence of the inlet field (IF) in the source region was also examined. All of these studies led to the determination of the optimal analytical parameters as well as to a better understanding of the initial ion cloud anatomy.
The analytical performance of the spectrometer was then studied. Limits of detection (LOD) and linear ranges were determined under static and pulsed ion injection conditions and interpreted in the context of the IR-MALDI mechanism. Applications in the separation of simple mixtures were also illustrated, demonstrating good isomer separation capabilities and the advantages of singly charged peaks. The possibility to couple high performance liquid chromatography (HPLC) to IR-MALDI-IM spectrometry was also demonstrated. Finally, the reduced pressure spectrometer was used to study the effect of high reduced field strength on the mobility of polyatomic ions in polyatomic gases.
The last focus point was on the study of peptide ions. A dataset obtained with electrospray IM spectrometry was characterized and used for the calibration of a collision cross-section (CCS) determination method based on molecular dynamics (MD) simulations at high temperature. Instead of producing candidate structures which are evaluated one by one, this semi-automated method uses the simulation as a whole to determine a single average collision cross-section value by reweighting the CCS of a few representative structures. The method was compared to the intrinsic size parameter (ISP) method and to experimental results. Additional MD data obtained from the simulations was also used to further analyze the peptides and understand the experimental results, an advantage with regard to the ISP method. Finally, the CCS of peptide ions analyzed by IR-MALDI were also evaluated with both ISP and MD methods and the results compared to experiment, resulting in a first validation of the MD method. Thus, this thesis brings together the soft ionization technique that is IR-MALDI, which produces mostly singly charged peaks, with ion mobility spectrometry, which can distinguish between isomers, and a collision cross-section determination method which also provides structural information on the analyte at hand.
Previous studies on native language (L1) anaphor resolution have found that monolingual native speakers are sensitive to syntactic, pragmatic, and semantic constraints on pronouns and reflexive resolution. However, most studies have focused on English and other Germanic languages, and little is currently known about the online (i.e., real-time) processing of anaphors in languages with syntactically less restricted anaphors, such as Turkish. We also know relatively little about how 'non-standard' populations such as non-native (L2) speakers and heritage speakers (HSs) resolve anaphors.
This thesis investigates the interpretation and real-time processing of anaphors in German and in a typologically different and as yet understudied language, Turkish. It compares hypotheses about differences between native speakers' (L1ers) and L2 speakers' (L2ers) sentence processing, looking into differences in processing mechanisms as well as the possibility of cross-linguistic influence. To help fill the current research gap regarding HS sentence comprehension, it compares findings for this group with those for L2ers.
To investigate the representation and processing of anaphors in these three populations, I carried out a series of offline questionnaires and Visual-World eye-tracking experiments on the resolution of reflexives and pronouns in both German and Turkish. In the German experiments, native German speakers as well as L2ers of German were tested, while in the Turkish experiments, non-bilingual native Turkish speakers as well as HSs of Turkish with L2 German were tested. This allowed me to observe both cross-linguistic differences as well as population differences between monolinguals' and different types of bilinguals' resolution of anaphors.
Regarding the comprehension of Turkish anaphors by L1ers, contrary to what has been previously assumed, I found that Turkish has no reflexive that follows Condition A of Binding theory (Chomsky, 1981). Furthermore, I propose more general cross-linguistic differences between Turkish and German, in the form of a stronger reliance on pragmatic information in anaphor resolution overall in Turkish compared to German.
As for the processing differences between L1ers and L2ers of a language, I found evidence in support of hypotheses which propose that L2ers of German rely more strongly on non-syntactic information compared to L1ers (Clahsen & Felser, 2006, 2017; Cunnings, 2016, 2017) independent of a potential influence of their L1. HSs, on the other hand, showed a tendency to overemphasize interpretational contrasts between different Turkish anaphors compared to monolingual native speakers. However, lower-proficiency HSs were likely to merge different forms for simplified representation and processing. Overall, L2ers and HSs showed differences from monolingual native speakers both in their final interpretation of anaphors and during online processing. However, these differences were not parallel between the two types of bilingual and thus do not support a unified model of L2 and HS processing (cf. Montrul, 2012).
The findings of this thesis contribute to the field of anaphor resolution by providing data from a previously unexplored language, Turkish, as well as contributing to research on native and non-native processing differences. My results also illustrate the importance of considering individual differences in the acquisition process when studying bilingual language comprehension. Factors such as age of acquisition, language proficiency and the type of input a language learner receives may influence the processing mechanisms they develop and employ, both between and within different bilingual populations.
Together with the gradual change of mean values, ongoing climate change is projected to increase frequency and amplitude of temperature and precipitation extremes in many regions of Europe. The impacts of such in most cases short term extraordinary climate situations on terrestrial ecosystems are a matter of central interest of recent climate change research, because it can not per se be assumed that known dependencies between climate variables and ecosystems are linearly scalable. So far, yet, there is a high demand for a method to quantify such impacts in terms of simultaneities of event time series.
In the course of this manuscript the new statistical approach of Event Coincidence Analysis (ECA) as well as it's R implementation is introduced, a methodology that allows assessing whether or not two types of event time series exhibit similar sequences of occurrences. Applications of the method are presented, analyzing climate impacts on different temporal and spacial scales: the impact of extraordinary expressions of various climatic variables on tree stem variations (subdaily and local scale), the impact of extreme temperature and precipitation events on the owering time of European shrub species (weekly and country scale), the impact of extreme temperature events on ecosystem health in terms of NDVI (weekly and continental scale) and the impact of El Niño and La Niña events on precipitation anomalies (seasonal and global scale).
The applications presented in this thesis refine already known relationships based on classical methods and also deliver substantial new findings to the scientific community: the widely known positive correlation between flowering time and temperature for example is confirmed to be valid for the tails of the distributions while the widely assumed positive dependency between stem diameter variation and temperature is shown to be not valid for very warm and very cold days. The larger scale investigations underline the sensitivity of anthrogenically shaped landscapes towards temperature extremes in Europe and provide a comprehensive global ENSO impact map for strong precipitation events.
Finally, by publishing the R implementation of the method, this thesis shall enable other researcher to further investigate on similar research questions by using Event Coincidence Analysis.
Answer Set Programming (ASP) is a declarative problem solving approach, combining a rich yet simple modeling language with high-performance solving capabilities. Although this has already resulted in various applications, certain aspects of such applications are more naturally modeled using variables over finite domains, for accounting for resources, fine timings, coordinates, or functions. Our goal is thus to extend ASP with constraints over integers while preserving its declarative nature. This allows for fast prototyping and elaboration tolerant problem descriptions of resource related applications. The resulting paradigm is called Constraint Answer Set Programming (CASP).
We present three different approaches for solving CASP problems. The first one, a lazy, modular approach combines an ASP solver with an external system for handling constraints. This approach has the advantage that two state of the art technologies work hand in hand to solve the problem, each concentrating on its part of the problem. The drawback is that inter-constraint dependencies cannot be communicated back to the ASP solver, impeding its learning algorithm. The second approach translates all constraints to ASP. Using the appropriate encoding techniques, this results in a very fast, monolithic system. Unfortunately, due to the large, explicit representation of constraints and variables, translation techniques are restricted to small and mid-sized domains. The third approach merges the lazy and the translational approach, combining the strength of both while removing their weaknesses. To this end, we enhance the dedicated learning techniques of an ASP solver with the inferences of the translating approach in a lazy way. That is, the important knowledge is only made explicit when needed.
By using state of the art techniques from neighboring fields, we provide ways to tackle real world, industrial size problems. By extending CASP to reactive solving, we open up new application areas such as online planning with continuous domains and durations.
The development of self-adaptive software requires the engineering of an adaptation engine that controls the underlying adaptable software by a feedback loop. State-of-the-art approaches prescribe the feedback loop in terms of numbers, how the activities (e.g., monitor, analyze, plan, and execute (MAPE)) and the knowledge are structured to a feedback loop, and the type of knowledge. Moreover, the feedback loop is usually hidden in the implementation or framework and therefore not visible in the architectural design. Additionally, an adaptation engine often employs runtime models that either represent the adaptable software or capture strategic knowledge such as reconfiguration strategies. State-of-the-art approaches do not systematically address the interplay of such runtime models, which would otherwise allow developers to freely design the entire feedback loop.
This thesis presents ExecUtable RuntimE MegAmodels (EUREMA), an integrated model-driven engineering (MDE) solution that rigorously uses models for engineering feedback loops. EUREMA provides a domain-specific modeling language to specify and an interpreter to execute feedback loops. The language allows developers to freely design a feedback loop concerning the activities and runtime models (knowledge) as well as the number of feedback loops. It further supports structuring the feedback loops in the adaptation engine that follows a layered architectural style. Thus, EUREMA makes the feedback loops explicit in the design and enables developers to reason about design decisions.
To address the interplay of runtime models, we propose the concept of a runtime megamodel, which is a runtime model that contains other runtime models as well as activities (e.g., MAPE) working on the contained models. This concept is the underlying principle of EUREMA. The resulting EUREMA (mega)models are kept alive at runtime and they are directly executed by the EUREMA interpreter to run the feedback loops. Interpretation provides the flexibility to dynamically adapt a feedback loop. In this context, EUREMA supports engineering self-adaptive software in which feedback loops run independently or in a coordinated fashion within the same layer as well as on top of each other in different layers of the adaptation engine. Moreover, we consider preliminary means to evolve self-adaptive software by providing a maintenance interface to the adaptation engine.
This thesis discusses in detail EUREMA by applying it to different scenarios such as single, multiple, and stacked feedback loops for self-repairing and self-optimizing the mRUBiS application. Moreover, it investigates the design and expressiveness of EUREMA, reports on experiments with a running system (mRUBiS) and with alternative solutions, and assesses EUREMA with respect to quality attributes such as performance and scalability.
The conducted evaluation provides evidence that EUREMA as an integrated and open MDE approach for engineering self-adaptive software seamlessly integrates the development and runtime environments using the same formalism to specify and execute feedback loops, supports the dynamic adaptation of feedback loops in layered architectures, and achieves an efficient execution of feedback loops by leveraging incrementality.
The sequencing of the human genome in the early 2000s led to an increased interest in cheap and fast sequencing technologies. This interest culminated in the advent of next generation sequencing (NGS). A number of different NGS platforms have arisen since then all promising to do the same thing, i.e. produce large amounts of genetic information for relatively low costs compared to more traditional methods such as Sanger sequencing. The capabilities of NGS meant that researchers were no longer bound to species for which a lot of previous work had already been done (e.g. model organisms and humans) enabling a shift in research towards more novel and diverse species of interest. This capability has greatly benefitted many fields within the biological sciences, one of which being the field of evolutionary biology. Researchers have begun to move away from the study of laboratory model organisms to wild, natural populations and species which has greatly expanded our knowledge of evolution. NGS boasts a number of benefits over more traditional sequencing approaches. The main benefit comes from the capability to generate information for drastically more loci for a fraction of the cost. This is hugely beneficial to the study of wild animals as, even when large numbers of individuals are unobtainable, the amount of data produced still allows for accurate, reliable population and species level results from a small selection of individuals.
The use of NGS to study species for which little to no previous research has been carried out on and the production of novel evolutionary information and reference datasets for the greater scientific community were the focuses of this thesis. Two studies in this thesis focused on producing novel mitochondrial genomes from shotgun sequencing data through iterative mapping, bypassing the need for a close relative to serve as a reference sequence. These mitochondrial genomes were then used to infer species level relationships through phylogenetic analyses. The first of these studies involved reconstructing a complete mitochondrial genome of the bat eared fox (Otocyon megalotis). Phylogenetic analyses of the mitochondrial genome confidently placed the bat eared fox as sister to the clade consisting of the raccoon dog and true foxes within the canidae family. The next study also involved reconstructing a mitochondrial genome but in this case from the extinct Macrauchenia of South America. As this study utilised ancient DNA, it involved a lot of parameter testing, quality controls and strict thresholds to obtain a near complete mitochondrial genome devoid of contamination known to plague ancient DNA studies. Phylogenetic analyses confidently placed Macrauchenia as sister to all living representatives of Perissodactyla with a divergence time of ~66 million years ago. The third and final study of this thesis involved de novo assemblies of both nuclear and mitochondrial genomes from brown and striped hyena and focussed on demographic, genetic diversity and population genomic analyses within the brown hyena. Previous studies of the brown hyena hinted at very low levels of genomic diversity and, perhaps due to this, were unable to find any notable population structure across its range. By incorporating a large number of genetic loci, in the form of complete nuclear genomes, population structure within the brown hyena was uncovered. On top of this, genomic diversity levels were compared to a number of other species. Results showed the brown hyena to have the lowest genomic diversity out of all species included in the study which was perhaps caused by a continuous and ongoing decline in effective population size that started about one million years ago and dramatically accelerated towards the end of the Pleistocene.
The studies within this thesis show the power NGS sequencing has and its utility within evolutionary biology. The most notable capabilities outlined in this thesis involve the study of species for which no reference data is available and in the production of large amounts of data, providing evolutionary answers at the species and population level that data produced using more traditional techniques simply could not.
Business process management is an acknowledged asset for running an organization in a productive and sustainable way. One of the most important aspects of business process management, occurring on a daily basis at all levels, is decision making. In recent years, a number of decision management frameworks have appeared in addition to existing business process management systems. More recently, Decision Model and Notation (DMN) was developed by the OMG consortium with the aim of complementing the widely used Business Process Model and Notation (BPMN). One of the reasons for the emergence of DMN is the increasing interest in the evolving paradigm known as the separation of concerns. This paradigm states that modeling decisions complementary to processes reduces process complexity by externalizing decision logic from process models and importing it into a dedicated decision model. Such an approach increases the agility of model design and execution. This provides organizations with the flexibility to adapt to the ever increasing rapid and dynamic changes in the business ecosystem. The research gap, identified by us, is that the separation of concerns, recommended by DMN, prescribes the externalization of the decision logic of process models in one or more separate decision models, but it does not specify this can be achieved.
The goal of this thesis is to overcome the presented gap by developing a framework for discovering decision models in a semi-automated way from information about existing process decision making. Thus, in this thesis we develop methodologies to extract decision models from: (1) control flow and data of process models that exist in enterprises; and (2) from event logs recorded by enterprise information systems, encapsulating day-to-day operations. Furthermore, we provide an extension of the methodologies to discover decision models from event logs enriched with fuzziness, a tool dealing with partial knowledge of the process execution information. All the proposed techniques are implemented and evaluated in case studies using real-life and synthetic process models and event logs. The evaluation of these case studies shows that the proposed methodologies provide valid and accurate output decision models that can serve as blueprints for executing decisions complementary to process models. Thus, these methodologies have applicability in the real world and they can be used, for example, for compliance checks, among other uses, which could improve the organization's decision making and hence it's overall performance.
Active and passive source data from two seismic experiments within the interdisciplinary project TIPTEQ (from The Incoming Plate to mega Thrust EarthQuake processes) were used to image and identify the structural and petrophysical properties (such as P- and S-velocities, Poisson's ratios, pore pressure, density and amount of fluids) within the Chilean seismogenic coupling zone at 38.25°S, where in 1960 the largest earthquake ever recorded (Mw 9.5) occurred. Two S-wave velocity models calculated using traveltime and noise tomography techniques were merged with an existing velocity model to obtain a 2D S-wave velocity model, which gathered the advantages of each individual model. In a following step, P- and S-reflectivity images of the subduction zone were obtained using different pre stack and post-stack depth migration techniques. Among them, the recent prestack line-drawing depth migration scheme yielded revealing results. Next, synthetic seismograms modelled using the reflectivity method allowed, through their input 1D synthetic P- and S-velocities, to infer the composition and rocks within the subduction zone. Finally, an image of the subduction zone is given, jointly interpreting the results from this work with results from other studies. The Chilean seismogenic coupling zone at 38.25°S shows a continental crust with highly reflective horizontal, as well as (steep) dipping events. Among them, the Lanalhue Fault Zone (LFZ), which is interpreted to be east-dipping, is imaged to very shallow depths. Some steep reflectors are observed for the first time, for example one near the coast, related to high seismicity and another one near the LFZ. Steep shallow reflectivity towards the volcanic arc could be related to a steep west-dipping reflector interpreted as fluids and/or melts, migrating upwards due to material recycling in the continental mantle wedge. The high resolution of the S-velocity model in the first kilometres allowed to identify several sedimentary basins, characterized by very low P- and S-velocities, high Poisson's ratios and possible steep reflectivity. Such high Poisson's ratios are also observed within the oceanic crust, which reaches the seismogenic zone hydrated due to bending-related faulting. It is interpreted to release water until reaching the coast and under the continental mantle wedge. In terms of seismic velocities, the inferred composition and rocks in the continental crust is in agreement with field geology observations at the surface along the proflle. Furthermore, there is no requirement to call on the existence of measurable amounts of present-day fluids above the plate interface in the continental crust of the Coastal Cordillera and the Central Valley in this part of the Chilean convergent margin. A large-scale anisotropy in the continental crust and upper mantle, previously proposed from magnetotelluric studies, is proposed from seismic velocities. However, quantitative studies on this topic in the continental crust of the Chilean seismogenic zone at 38.25°S do not exist to date.
Earth's climate varies continuously across space and time, but humankind has witnessed only a small snapshot of its entire history, and instrumentally documented it for a mere 200 years. Our knowledge of past climate changes is therefore almost exclusively based on indirect proxy data, i.e. on indicators which are sensitive to changes in climatic variables and stored in environmental archives. Extracting the data from these archives allows retrieval of the information from earlier times. Obtaining accurate proxy information is a key means to test model predictions of the past climate, and only after such validation can the models be used to reliably forecast future changes in our warming world. The polar ice sheets of Greenland and Antarctica are one major climate archive, which record information about local air temperatures by means of the isotopic composition of the water molecules embedded in the ice. However, this temperature proxy is, as any indirect climate data, not a perfect recorder of past climatic variations. Apart from local air temperatures, a multitude of other processes affect the mean and variability of the isotopic data, which hinders their direct interpretation in terms of climate variations. This applies especially to regions with little annual accumulation of snow, such as the Antarctic Plateau. While these areas in principle allow for the extraction of isotope records reaching far back in time, a strong corruption of the temperature signal originally encoded in the isotopic data of the snow is expected. This dissertation uses observational isotope data from Antarctica, focussing especially on the East Antarctic low-accumulation area around the Kohnen Station ice-core drilling site, together with statistical and physical methods, to improve our understanding of the spatial and temporal isotope variability across different scales, and thus to enhance the applicability of the proxy for estimating past temperature variability. The presented results lead to a quantitative explanation of the local-scale (1–500 m) spatial variability in the form of a statistical noise model, and reveal the main source of the temporal variability to be the mixture of a climatic seasonal cycle in temperature and the effect of diffusional smoothing acting on temporally uncorrelated noise. These findings put significant limits on the representativity of single isotope records in terms of local air temperature, and impact the interpretation of apparent cyclicalities in the records. Furthermore, to extend the analyses to larger scales, the timescale-dependency of observed Holocene isotope variability is studied. This offers a deeper understanding of the nature of the variations, and is crucial for unravelling the embedded true temperature variability over a wide range of timescales.
Microswimmers, i.e. swimmers of micron size experiencing low Reynolds numbers, have received a great deal of attention in the last years, since many applications are envisioned in medicine and bioremediation. A promising field is the one of magnetic swimmers, since magnetism is biocom-patible and could be used to direct or actuate the swimmers. This thesis studies two examples of magnetic microswimmers from a physics point of view.
The first system to be studied are magnetic cells, which can be magnetic biohybrids (a swimming cell coupled with a magnetic synthetic component) or magnetotactic bacteria (naturally occurring bacteria that produce an intracellular chain of magnetic crystals). A magnetic cell can passively interact with external magnetic fields, which can be used for direction. The aim of the thesis is to understand how magnetic cells couple this magnetic interaction to their swimming strategies, mainly how they combine it with chemotaxis (the ability to sense external gradient of chemical species and to bias their walk on these gradients). In particular, one open question addresses the advantage given by these magnetic interactions for the magnetotactic bacteria in a natural environment, such as porous sediments. In the thesis, a modified Active Brownian Particle model is used to perform simulations and to reproduce experimental data for different systems such as bacteria swimming in the bulk, in a capillary or in confined geometries. I will show that magnetic fields speed up chemotaxis under special conditions, depending on parameters such as their swimming strategy (run-and-tumble or run-and-reverse), aerotactic strategy (axial or polar), and magnetic fields (intensities and orientations), but it can also hinder bacterial chemotaxis depending on the system.
The second example of magnetic microswimmer are rigid magnetic propellers such as helices or random-shaped propellers. These propellers are actuated and directed by an external rotating magnetic field. One open question is how shape and magnetic properties influence the propeller behavior; the goal of this research field is to design the best propeller for a given situation. The aim of the thesis is to propose a simulation method to reproduce the behavior of experimentally-realized propellers and to determine their magnetic properties. The hydrodynamic simulations are based on the use of the mobility matrix. As main result, I propose a method to match the experimental data, while showing that not only shape but also the magnetic properties influence the propellers swimming characteristics.
This project was focused on exploring the phase behavior of poly(styrene)187000-block-poly(2-vinylpyridine)203000 (SV390) with high molecular weight (390 kg/mol) in thin films, in which the self-assembly of block copolymers (BCPs) was realized via thermo-solvent annealing. The advanced processing technique of solvent vapor treatment provides controlled and stable conditions.
In Chapter 3, the factors to influence the annealing process and the swelling behavior of homopolymers are presented and discussed. The swelling behavior of BCP in films is controlled by the temperature of the vapor and of the substrate, on one hand, and variation of the saturation of the solvent vapor atmosphere (different solvents), on the other hand. Additional factors like the geometry and material of the chamber, the type of flow inside the chamber etc. also influence the reproducibility and stability of the processing. The slightly selective solvent vapor of chloroform gives 10% more swelling of P2VP than PS in films with thickness of ~40 nm.
The tunable morphology in ultrathin films of high molecular weight BCP (SV390) was investigated in Chapter 4. First, the swelling behavior can be precisely tuned by temperature and/or vapor flow separately, which provided information for exploring the multiple-parameter-influenced segmental chain mobility of polymer films. The equilibrium state of SV390 in thin films influenced by temperature was realized at various temperatures with the same degree of swelling. Various methods including characterization with SFM, metallization and RIE were used to identify the morphology of films as porous half-layer with PS dots and P2VP matrix. The kinetic investigations demonstrate that on substrates with either weak or strong interaction the original morphology of the BCP with high molecular weight is changed very fast within 5 min, and the further annealing serves for annihilation of defects.
The morphological development of symmetric BCP in films with thickness increasing from half-layer to one-layer influenced by confinement factors of gradient film thicknesses and various surface properties of substrates was studied in Chapter 5. SV390 and SV99 films show bulk lamella-forming morphology after slightly selective solvent vapor (chloroform) treatment. SV99 films show cylinder-forming morphology under strongly selective solvent vapor (toluene) treatment since the asymmetric structure (caused by toluene uptake in PS blocks only) of SV99 block copolymer during annealing. Both kinds of morphology (lamella and cylinder) are influenced by the film thickness. The annealed morphology of SV390 and SV99 influenced by the combination of confined film and substrate property is similar to the morphology on flat silicon wafers. In this chapter the gradients in the film thickness and surface properties of the substrates with regard to their influence on the morphological development in thin BCP films are presented. Directed self-assembly (graphoepitaxy) of this SV390 was also investigated to compare with systematically reported SV99.
In Chapter 6 an approach to induced oriented microphase separation in thick block copolymer films via treatment with the oriented vapor flow using mini-extruder is envisaged to be an alternative to existing methodologies, e.g. via non-solvent-induced phase separation. The preliminary tests performed in this study confirm potential perspective of this method, which alters the structure through the bulk of the film (as revealed by SAXS measurements), but more detailed studies have to be conducted in order to optimize the preparation.
BACKGROUND: Physical activity involving high spinal load has been exposed to possess a crucial impact in the genesis of acute and chronic low back pain and disorder. Vigorous spinal loads are surmised in drop landings, for which strenuous bending loads were formerly evinced for the lower extremity structures. Thus far, clinical studies revealed that repetitive landing impacts can evoke benign structural adaptions or damage to the lumbar vertebrae. Though, causes for these observations are hitherto not conclusively evinced; since actual spinal load has to date not been experimentally documented. Moreover, it is yet undetermined how physiological activation of trunk musculature compensates for landing impact induced spinal loads, and to which extend trunk activity and spinal load are affected by landing demands and performer characteristics. AIMS of this study are 1. the localisation and quantification of spinal bending loads under various landing demands and 2. the identification of compensatory trunk muscular activity pattern, which potentially alleviate spinal load magnitudes. Three consecutive Hypotheses (H1 - H3) were hereto postulated: H1 posits that spinal bending loads in segregated motion planes can feasibly and reliably be evaluated from peak spine segmental angular accelerations. H2 furthermore assumes that vertical drop landings elicit highest spine bending load in sagittal flexion of the lumbar spine. Based on these verifications, a second study shall prove the successive hypothesis (H3) that diversified landing conditions, like performer’s landing familiarity and gender, as an implementation of an instantaneous follow-up task, affect the emerging lumbar spinal bending load. Herein it is moreover surmised that lumbar spinal bending loads under distinct landing conditions are predominantly modulated by herewith disparately deployed conditioned pre-activations of trunk muscles. METHODS: To test the above arrayed hypothesis, two successive studies were carried out. In STUDY 1, 17 subjects were repetitively assessed performing various drop landings (heigth: 15, 30, 45, 60cm; unilateral, bilateral, blindfolded, catching a ball) in a test-retest-design. Herein individual peak angular accelerations [αMAX] were derived from three-dimensional motion data of four trunk-segments (upper thoracic, lower thoracic, lumbar, pelvis). αMAX was herein assessed in flexion, lateral flexion, and rotation of each spinal joint, formed by two adjacent segments. Reliability of αMAX within and between test-days was evaluated by CV%, ICC 2.1, TRV%, and Bland & Altman Analysis (BIAS±LoA). Subsequently, peak flexion acceleration of the lumbo-pelvic joint [αFLEX[LS-PV]] was statistically compared to αMAX expressions of each other assessed spinal joint and motion plane (Mean ±SD, Independent Samples T-test). STUDY 2 deliberately assessed mere peak lumbo-pelvic flexion accelerations [αFLEX[LS-PV]] and electro-myographic trunk pre-activity prior to αFLEX[LS-PV] on 43 subjects performing varied landing tasks (height 45cm; with definite or indefinite predictability of a subsequent instant follow up jump). Subjects were contrasted with respect to their previous landing familiarity ( >1000 vs. <100 landings performed in the past 10 years) and gender. Differences of αFLEX[LS-PV] and muscular pre-activity between contrasted subject groups as between landing tasks were equally statistically tested by three-way mixed ANOVA with Post-hoc tests. Associations between αFLEX[LS-PV] and muscular pre-activity were factor-specifically assessed by Spearman’s rank order correlation coefficient (rS). Complementarily, muscular pre-activity was subdivided by landing phases [DROP, IMPACT] and discretely assessed for phase specific associations to αFLEX[LS-PV]. Each muscular activity was moreover pairwise compared between DROP and IMPACT (Mean ±SD, Dependent Samples T-test). RESULTS: αMAX was presented with overall high variability within test-days (CV =36%). Lowest intra-individual variability and highest reproducibility of αMAX between test-days was shown in flexion of the spine. αFLEX[LS-PV] showed largely consistent sig. higher magnitudes compared to αMAX presented in more cranial spinal joints and other motion planes. αFLEX[LS-PV] moreover gradually increased with escalations in landing heights. Landing unfamiliar subjects presented sig. higher αFLEX[LS-PV] in contrast to landing familiar ones (p=.016). M. Obliquus Int. with M. Transversus Abd. (66 ±32%MVC) and M. Erector Spinae (47 ±15%MVC) presented maredly highest activity in contrast to lowest activity of M. Rectus Abd. (10 ±4%MVC). Landing unfamiliar subjects showed compared to landing familiar ones sig. higher activity of M. Obliquus Ext. (17 ±8%MVC, 12 ±7%MVC, p= .044). M. Obliquus Ext. and its co-contraction ratio with M. Erector Spinae moreover exhibited low but sig. positive correlations to αFLEX[LS-PV] (rs=.39, rs=.31). Each trunk muscule distributed larger shares of its activity to DROP, whereas peak activations of most muscles emerged in the proportionally shorter IMPACT phase. Commonly increased muscular pre-activation particularly at IMPACT was found in landings with a contrived follow up jump and in female subjects, whereby αFLEX[LS-PV] was hereof only marginally affected. DISCUSSION: Highest spine segmental angular accelerations in drop landings emerge in sagittal flexion of the lumbar spine. The compensatory stabilisation of the spine appears to be preponderantly provided by a dorso-ventral co-contraction of M. Obliquus Int., M. Transversus Abd. and M. Erector Spinae. Elevated pre-activity of M. Obliquuis Ext. supposably characterises poor landing experience, which might engender increased bending loads to the lumbar spine. A pervasive large variability of spinal angular accelerations measured across all landing types, suggests a multifarious utilisation of diverse mechanisms compensating for spinal impacts in landing performances. A standardised assessment and valid evaluation of landing evoked lumbar bending loads is hereof largley confined. CONCLUSION: Drop landings elicit most strenuous lumbo-pelvic flexion accelerations, which can be appraised as representatives for high energetic bending loads to the spine. Such entail the highest risk to overload the spinal tissue, when landing demands exceed the individual’s landing skill. Previous landing experience and training appears to effectively improve muscular spine stabilisation pattern, diminishing spinal bending loads.
East Africa is a natural laboratory: Studying its unique geological and biological history can help us better inform our theories and models. Studying its present and future can help us protect its globally important biodiversity and ecosystem services. East African vegetation plays a central role in all these aspects, and this dissertation aims to quantify its dynamics through computer simulations.
Computer models help us recreate past settings, forecast into the future or conduct simulation experiments that we cannot otherwise perform in the field. But before all that, one needs to test their performance. The outputs that the model produced using the present day-inputs, agreed well with present-day observations of East African vegetation. Next, I simulated past vegetation for which we have fossil pollen data to compare. With computer models, we can fill the gaps of knowledge between sites where we have fossil pollen data from, and create a more complete picture of the past. Good level of agreement between model and pollen data where they overlapped in space further validated our model performance.
Once the model was tested and validated for the region, it became possible to probe one of the long standing questions regarding East African vegetation: How did East Africa lose its tropical forests? The present-day vegetation in the tropics is mainly characterized by continuous forests worldwide except in tropical East Africa, where forests only occur as patches. In a series of simulation experiments, I was able to show under which conditions these forest patches could have been connected and fragmented in the past. This study showed the sensitivity of East African vegetation to climate change and variability such as those expected under future climate change.
El Niño Southern Oscillation (ENSO) events that result from the fluctuations in temperature between the ocean and atmosphere, bring further variability to East African climate and are predicted to increase in intensity in the future. But climate models are still not good at capturing the pattens of these events. In a study where I quantified the influence of ENSO events on East African vegetation, I showed how different the future vegetation could be from what we currently predict with these climate models that lack accurate ENSO contribution. Consideration of these discrepancies is important for our future global carbon budget calculations and management decisions.
Ferroic materials have attracted a lot of attention over the years due to their wide range of applications in sensors, actuators, and memory devices. Their technological applications originate from their unique properties such as ferroelectricity and piezoelectricity. In order to optimize these materials, it is necessary to understand the coupling between their nanoscale structure and transient response, which are related to the atomic structure of the unit cell.
In this thesis, synchrotron X-ray diffraction is used to investigate the structure of ferroelectric thin film capacitors during application of a periodic electric field. Combining electrical measurements with time-resolved X-ray diffraction on a working device allows for visualization of the interplay between charge flow and structural motion. This constitutes the core of this work. The first part of this thesis discusses the electrical and structural dynamics of a ferroelectric Pt/Pb(Zr0.2,Ti0.8)O3/SrRuO3 heterostructure during charging, discharging, and polarization reversal. After polarization reversal a non-linear piezoelectric response develops on a much longer time scale than the RC time constant of the device. The reversal process is inhomogeneous and induces a transient disordered domain state. The structural dynamics under sub-coercive field conditions show that this disordered domain state can be remanent and can be erased with an appropriate voltage pulse sequence. The frequency-dependent dynamic characterization of a Pb(Zr0.52,Ti0.48)O3 layer, at the morphotropic phase boundary, shows that at high frequency, the limited domain wall velocity causes a phase lag between the applied field and both the structural and electrical responses. An external modification of the RC time constant of the measurement delays the switching current and widens the electromechanical hysteresis loop while achieving a higher compressive piezoelectric strain within the crystal.
In the second part of this thesis, time-resolved reciprocal space maps of multiferroic BiFeO3 thin films were measured to identify the domain structure and investigate the development of an inhomogeneous piezoelectric response during the polarization reversal. The presence of 109° domains is evidenced by the splitting of the Bragg peak.
The last part of this work investigates the effect of an optically excited ultrafast strain or heat pulse propagating through a ferroelectric BaTiO3 layer, where we observed an additional current response due to the laser pulse excitation of the metallic bottom electrode of the heterostructure.
Synthesis of artificial building blocks for sortase-mediated ligation and their enzymatic linkage
(2018)
The enzyme Sortase A catalyzes the formation of a peptide bond between the recognition sequence LPXTG and an oligoglycine. While manifold ligations between proteins and various biomolecules, proteins and small synthetic molecules as well as proteins and surfaces have been reported, the aim of this thesis was to investigate the sortase-catalyzed linkage between artificial building blocks. Hence, this could pave the way for the use of sortase A for tasks from a chemical point of view and maybe even materials science.
For the proof of concept, the studied systems were kept as simple as possible at first by choosing easily accessible silica NPs and commercially available polymers. These building blocks were functionalized with peptide motifs for sortase-mediated ligation. Silica nanoparticles were synthesized with diameters of 60 and 200 nm and surface modified with C=C functionalities. Then, peptides bearing a terminal cysteine were covalently linked by means of a thiol-ene reaction. 60 nm SiO2 NPs were functionalized with pentaglycines, while peptides with LPETG motif were linked to 200 nm silica particles. Polyethyleneglycol (PEG) and poly(N isopropylacrylamide) (PNIPAM) were likewise functionalized with peptides by thiol-ene reaction between cysteine residues and C=C units in the polymer end groups. Hence, G5-PEG and PNIPAM-LPETG conjugates were obtained. With this set of building blocks, NP–polymer hybrids, NP–NP, and polymer–polymer structures were generated by sortase-mediated ligation and the product formation shown by transmission electron microscopy, MALDI-ToF mass spectrometry and dynamic light scatting, among others. Thus, the linkage of these artificial building blocks by the enzyme sortase A could be demonstrated.
However, when using commercially available polymers, the purification of the polymer–peptide conjugates was impossible and resulted in a mixture containing unmodified polymer. Therefore, strategies were developed for the own synthesis of pure peptide-polymer and polymer-peptide conjugates as building blocks for sortase-mediated ligation. The designed routes are based on preparing polymer blocks via RAFT polymerization from CTAs that are attached to N- or C-terminus, respectively, of a peptide. GG-PNIPAM was synthesized through attachment of a suitable RAFT CTA to Fmoc-GG in an esterification reaction, followed by polymerization of NIPAM and cleavage of the Fmoc protection group. Furthermore, several peptides were synthesized by solid-phase peptide synthesis. The linkage of a RAFT CTA (or
polymerization initiator) to the N-terminus of a peptide can be conducted in an automated fashion as last step in a peptide synthesizer. The synthesis of such a conjugate couldn’t be realized in the time frame of this thesis, but many promising strategies exist to continue this strategy using different coupling reagents. Such polymer building blocks can be used to synthesize protein-polymer conjugates catalyzed by sortase A and the approach can be carried on to the synthesis of block copolymers by using polymer blocks with peptide motifs on both ends.
Although the proof of concept demonstrated in this thesis only shows examples that can be also synthesized by exclusively chemical techniques, a toolbox of such building blocks will enable the future formation of new materials and pave the way for the application of enzymes in materials science. In addition to nanoparticle systems and block copolymers, this also includes combination with protein-based building blocks to form hybrid materials. Hence, sortase could become an enzymatic tool that complements established chemical linking technologies and provides specific peptide motifs that are orthogonal to all existing chemical functional groups.
Thematic role assignment and word order preferences in the child language acquisition of Tagalog
(2018)
A critical task in daily communications is identifying who did what to whom in an utterance, or assigning the thematic roles agent and patient in a sentence. This dissertation is concerned with Tagalog-speaking children’s use of word order and morphosyntactic markers for thematic role assignment. It aims to explain children’s difficulties in interpreting sentences with a non-canonical order of arguments (i.e., patient-before-agent) by testing the predictions of the following accounts: the frequency account (Demuth, 1989), the Competition model (MacWhinney & Bates, 1989), and the incremental processing account (Trueswell & Gleitman, 2004). Moreover, the experiments in this dissertation test the influence of a word order strategy in a language like Tagalog, where the thematic roles are always unambiguous in a sentence, due to its verb-initial order and its voice-marking system. In Tagalog’s voice-marking system, the inflection on the verb indicates the thematic role of the noun marked by 'ang.' First, the possible basis for a word order strategy in Tagalog was established using a sentence completion experiment given to adults and 5- and 7-year-old children (Chapter 2) and a child-directed speech corpus analysis (Chapter 3). In general, adults and children showed an agent-before-patient preference, although adults’ preference was also affected by sentence voice. Children’s comprehension was then examined through a self-paced listening and picture verification task (Chapter 3) and an eye-tracking and picture selection task (Chapter 4), where word order (agent-initial or patient-initial) and voice (agent voice or patient voice) were manipulated. Offline (i.e., accuracy) and online (i.e., listening times, looks to the target) measures revealed that 5- and 7-year-old Tagalog-speaking children had a bias to interpret the first noun as the agent. Additionally, the use of word order and morphosyntactic markers was found to be modulated by voice. In the agent voice, children relied more on a word order strategy; while in the patient voice, they relied on the morphosyntactic markers. These results are only partially explained by the accounts being tested in this dissertation. Instead, the findings support computational accounts of incremental word prediction and learning such as Chang, Dell, & Bock’s (2006) model.
Future magnetic recording industry needs a high-density data storage technology. However, switching the magnetization of small bits requires high magnetic fields that cause excessive heat dissipation. Therefore, controlling magnetism without applying external magnetic field is an important research topic for potential applications in data storage devices with low power consumption. Among the different approaches being investigated, two of them stand out, namely i) all-optical helicity dependent switching (AO-HDS) and ii) ferroelectric control of magnetism. This thesis aims to contribute towards a better understanding of the physical processes behinds these effects as well as reporting new and exciting possibility for the optical and/or electric control of magnetic properties. Hence, the thesis contains two differentiated chapters of results; the first devoted to AO-HDS on TbFe alloys and the second to the electric field control of magnetism in an archetypal Fe/BaTiO3 system.
In the first part, the scalability of the AO-HDS to small laser spot-sizes of few microns in the ferrimagnetic TbFe alloy is investigated by spatially resolving the magnetic contrast with photo-emission electron microscopy (PEEM) and X-ray magnetic circular dichroism (XMCD). The results show that the AO-HDS is a local effect within the laser spot size that occurs in the ring-shaped region in the vicinity of thermal demagnetization. Within the ring region, the helicity dependent switching occurs via thermally activated domain wall motion. Further, the thesis reports on a novel effect of thickness dependent inversion of the switching orientation. It addresses some of the important questions like the role of laser heating and the microscopic mechanism driving AO-HDS.
The second part of the thesis focuses on the electric field control of magnetism in an artificial multiferroic heterostructure. The sample consists of an Fe wedge with thickness varying between 0:5 nm and 3 nm, deposited on top of a ferroelectric and ferroelastic BaTiO3 [001]-oriented single crystal substrate. Here, the magnetic contrast is imaged via PEEM and XMCD as a function of out-of-plane voltage. The results show the evidence of the electric field control of superparamagnetism mediated by a ferroelastic modification of the magnetic anisotropy. The changes in the magnetoelastic anisotropy drive the transition from the superparamagnetic to superferromagnetic state at localized sample positions.
Various ways of preparing enantiomerically pure 2-amino[6]helicene derivatives were explored. Ni(0) mediated cyclotrimerization of enantiopure triynes provided (M)- and (P)-7,8-bis(p-tolyl)hexahelicene-2-amine in >99% ee as well as its benzoderivative in >99% ee. The stereocontrol was found to be inefficient for a 2- aminobenzo[6]helicene congener with an embedded five-membered ring. Helically chiral imidazolium salts bearing one or two helicene moieties have been synthesized and applied in enantioselective [2+2+2] cyclotrimerization catalyzed by an in situ formed Ni(0)-NHC complex. The synthesis of the first helically chiral Pd- and Ru-NHC complexes and their application in enantioselective catalysis was demonstrated. The latter shows promising results in enantioselective olefin metathesis reactions. A mechanistic proposal for asymmetric ring closing metathesis is provided.
Eta Carinae
(2018)
The exceptional binary star Eta Carinae has been fascinating scientists and the people in the Southern hemisphere alike for hundreds of years. It survived an enormous outbreak, comparable to a supernova energy-wise, and for a short period became the brightest star of the night sky. From observations from the radio regime to X-rays the system's characteristics and its emission in photon energies up to ~ 50 keV are well studied today. The binary is composed of two massive stars of ~ 30 and ~ 100 solar masses. Either star drives a strong stellar wind that continuously carries away a fraction of its mass. The collision of these winds leads to a shock on each side of the encounter. In the wind-wind-collision region plasma gets heated when it is overrun by the shocks. Part of the emission seen in X-rays can be attributed to this plasma. Above ~ 50 keV the emission is no longer of thermal origin: the required plasma temperature exceeds the available mechanical energy input of the stellar winds. In contrast to its observational history in thermal energies observational evidence of Eta Carinae's non-thermal emission has only recently built up. In high-energy gamma-rays Eta Carinae is the only binary of its kind that has been detected unambiguously. Its energy spectrum reaches up to ~ hundred GeV, a regime where satellite-based gamma-ray experiments run out of statistics. Ground-based gamma-ray experiments have the advantage of large photon collection areas. H.E.S.S. is the only gamma-ray experiment located in the Southern hemisphere and thus able to observe Eta Carinae in this energy range. H.E.S.S. measures gamma-rays via electromagnetic showers of particles that very-high-energy gamma-rays initiate in the atmosphere. The main challenge in observations of Eta Carinae with H.E.S.S. is the UV emission of the Carina nebula that leads to a background that is up to 10 times stronger than usual for H.E.S.S. This thesis presents the first detection of a colliding-wind binary in very-high-energy gamma-rays and documents the studies that led to it. The differential gamma-ray energy spectrum of Eta Carinae is measured up to 700 GeV. A hadronic and leptonic origin of the gamma-ray emission is discussed and based on the comparison of cooling times a hadronic scenario is favoured.