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In this dissertation, an electric field-assisted method was developed and applied to achieve immobilization and alignment of biomolecules on metal electrodes in a simple one-step experiment. Neither modifications of the biomolecule nor of the electrodes were needed. The two major electrokinetic effects that lead to molecule motion in the chosen electrode configurations used were identified as dielectrophoresis and AC electroosmotic flow. To minimize AC electroosmotic flow, a new 3D electrode configuration was designed. Thus, the influence of experimental parameters on the dielectrophoretic force and the associated molecule movement could be studied. Permanent immobilization of proteins was examined and quantified absolutely using an atomic force microscope. By measuring the volumes of the immobilized protein deposits, a maximal number of proteins contained therein was calculated. This was possible since the proteins adhered to the tungsten electrodes even after switching off the electric field. The permanent immobilization of functional proteins on surfaces or electrodes is one crucial prerequisite for the fabrication of biosensors.
Furthermore, the biofunctionality of the proteins must be retained after immobilization. Due to the chemical or physical modifications on the proteins caused by immobilization, their biofunctionality is sometimes hampered. The activity of dielectrophoretically immobilized proteins, however, was proven here for an enzyme for the first time. The enzyme horseradish peroxidase was used exemplarily, and its activity was demonstrated with the oxidation of dihydrorhodamine 123, a non-fluorescent precursor of the fluorescence dye rhodamine 123.
Molecular alignment and immobilization - reversible and permanent - was achieved under the influence of inhomogeneous AC electric fields. For orientational investigations, a fluorescence microscope setup, a reliable experimental procedure and an evaluation protocol were developed and validated using self-made control samples of aligned acridine orange molecules in a liquid crystal.
Lambda-DNA strands were stretched and aligned temporarily between adjacent interdigitated electrodes, and the orientation of PicoGreen molecules, which intercalate into the DNA strands, was determined. Similarly, the aligned immobilization of enhanced Green Fluorescent Protein was demonstrated exploiting the protein's fluorescence and structural properties. For this protein, the angle of the chromophore with respect to the protein's geometrical axis was determined in good agreement with X-ray crystallographic data. Permanent immobilization with simultaneous alignment of the proteins was achieved along the edges, tips and on the surface of interdigitated electrodes. This was the first demonstration of aligned immobilization of proteins by electric fields.
Thus, the presented electric field-assisted immobilization method is promising with regard to enhanced antibody binding capacities and enzymatic activities, which is a requirement for industrial biosensor production, as well as for general interaction studies of proteins.
We elicited the production of various types of relative clauses in a group of German-speaking children with specific language impairment (SLI) and typically developing controls in order to test the movement optionality account of grammatical difficulty in SLI. The results show that German-speaking children with SLI are impaired in relative clause production compared to typically developing children. The alternative structures that they produce consist of simple main clauses, as well as nominal and prepositional phrases produced in isolation, sometimes contextually appropriate, and sometimes not. Crucially for evaluating the movement optionality account, children with SLI produce very few instances of embedded clauses where the relative clause head noun is pronounced in situ; in fact, such responses are more common among the typically developing child controls. These results underscore the difficulty German-speaking children with SLI have with structures involving movement, but provide no specific support for the movement optionality account.
En route towards advanced catalyst materials for the electrocatalytic water splitting reaction
(2016)
The thesis on hand deals with the development of new types of catalysts based on pristine metals and ceramic materials and their application as catalysts for the electrocatalytic water splitting reaction. In order to breathe life into this technology, cost-efficient, stable and efficient catalysts are imploringly desired. In this manner, the preparation of Mn-, N-, S-, P-, and C-containing nickel materials has been investigated together with the theoretical and electrochemical elucidation of their activity towards the hydrogen (and oxygen) evolution reaction. The Sabatier principle has been used as the principal guideline towards successful tuning of catalytic sites. Furthermore, two pathways have been chosen to ameliorate the electrocatalytic performance, namely, the direct improvement of intrinsic properties through appropriate material selection and secondly the increase of surface area of the catalytic material with an increased amount of active sites. In this manner, bringing materials with optimized hydrogen adsorption free energy onto high surface area support, catalytic performances approaching the golden standards of noble metals were feasible. Despite varying applied synthesis strategies (wet chemistry in organic solvents, ionothermal reaction, gas phase reaction), one goal has been systematically pursued: to understand the driving mechanism of the growth. Moreover, deeper understanding of inherent properties and kinetic parameters of the catalytic materials has been gained.
This article explores a recent performance of excerpts from T.S. Eliot’s Four Quartets (1935/36–1942) entitled Engaging Eliot: Four Quartets in Word, Color, and Sound as an example of live poetry. In this context, Eliot’s poem can be analysed as an auditory artefact that interacts strongly with other oral performances (welcome addresses and artists’ conversations), as well as with the musical performance of Christopher Theofanidis’s quintet “At the Still Point” at the end of the opening of Engaging Eliot. The event served as an introduction to a 13-day art exhibition and engaged in a re-evaluation of Eliot’s poem after 9/11: while its first part emphasises the connection between Eliot’s poem and Christian doctrine, its second part – especially the combination of poetry reading and musical performance – highlights the philosophical and spiritual dimensions of Four Quartets.
Arctic coastal infrastructure and cultural and archeological sites are increasingly vulnerable to erosion and flooding due to amplified warming of the Arctic, sea level rise, lengthening of open water periods, and a predicted increase in frequency of major storms. Mitigating these hazards necessitates decision-making tools at an appropriate scale. The objectives of this paper are to provide such a tool by assessing potential erosion and flood hazards at Herschel Island, a UNESCO World Heritage candidate site. This study focused on Simpson Point and the adjacent coastal sections because of their archeological, historical, and cultural significance. Shoreline movement was analyzed using the Digital Shoreline Analysis System (DSAS) after digitizing shorelines from 1952, 1970, 2000, and 2011. For purposes of this analysis, the coast was divided in seven coastal reaches (CRs) reflecting different morphologies and/or exposures. Using linear regression rates obtained from these data, projections of shoreline position were made for 20 and 50 years into the future. Flood hazard was assessed using a least cost path analysis based on a high-resolution light detection and ranging (LiDAR) dataset and current Intergovernmental Panel on Climate Change sea level estimates. Widespread erosion characterizes the study area. The rate of shoreline movement in different periods of the study ranges from −5.5 to 2.7 m·a⁻¹ (mean −0.6 m·a⁻¹). Mean coastal retreat decreased from −0.6 m·a⁻¹ to −0.5 m·a⁻¹, for 1952–1970 and 1970–2000, respectively, and increased to −1.3 m·a⁻¹ in the period 2000–2011. Ice-rich coastal sections most exposed to wave attack exhibited the highest rates of coastal retreat. The geohazard map combines shoreline projections and flood hazard analyses to show that most of the spit area has extreme or very high flood hazard potential, and some buildings are vulnerable to coastal erosion. This study demonstrates that transgressive forcing may provide ample sediment for the expansion of depositional landforms, while growing more susceptible to overwash and flooding.
Calcularis is a computer-based training program which focuses on basic numerical skills, spatial representation of numbers and arithmetic operations. The program includes a user model allowing flexible adaptation to the child's individual knowledge and learning profile. The study design to evaluate the training comprises three conditions (Calcularis group, waiting control group, spelling training group). One hundred and thirty-eight children from second to fifth grade participated in the study. Training duration comprised a minimum of 24 training sessions of 20 min within a time period of 6-8 weeks. Compared to the group without training (waiting control group) and the group with an alternative training (spelling training group), the children of the Calcularis group demonstrated a higher benefit in subtraction and number line estimation with medium to large effect sizes. Therefore, Calcularis can be used effectively to support children in arithmetic performance and spatial number representation.
Using an algorithm based on a retrospective rejection sampling scheme, we propose an exact simulation of a Brownian diffusion whose drift admits several jumps. We treat explicitly and extensively the case of two jumps, providing numerical simulations. Our main contribution is to manage the technical difficulty due to the presence of two jumps thanks to a new explicit expression of the transition density of the skew Brownian motion with two semipermeable barriers and a constant drift.
Much research on language control in bilinguals has relied on the interpretation of the costs of switching between two languages. Of the two types of costs that are linked to language control, switching costs are assumed to be transient in nature and modulated by trial-specific manipulations (e.g., by preparation time), while mixing costs are supposed to be more stable and less affected by trial-specific manipulations. The present study investigated the effect of preparation time on switching and mixing costs, revealing that both types of costs can be influenced by trial-specific manipulations.
Exhaustivity
(2016)
The dissertation proposes an answer to the question of how to model exhaustive inferences and what the meaning of the linguistic material that triggers these inferences is. In particular, it deals with the semantics of exclusive particles, clefts, and progressive aspect in Ga, an under-researched language spoken in Ghana. Based on new data coming from the author’s original fieldwork in Accra, the thesis points to a previously unattested variation in the semantics of exclusives in a cross-linguistic perspective, analyzes the connections between exhaustive interpretation triggered by clefts and the aspectual interpretation of the sentence, and identifies a cross-categorial definite determiner. By that it sheds new light on several exhaustivity-related phenomena in both the nominal and the verbal domain and shows that both domains are closely connected.
The aim of this thesis was the elucidation of different ionization methods (resonance-enhanced multiphoton ionization – REMPI, electrospray ionization – ESI, atmospheric pressure chemical ionization – APCI) in ion mobility (IM) spectrometry. In order to gain a better understanding of the ionization processes, several spectroscopic, mass spectrometric and theoretical methods were also used. Another focus was the development of experimental techniques, including a high resolution spectrograph and various combinations of IM and mass spectrometry.
The novel high resolution 2D spectrograph facilitates spectroscopic resolutions in the range of commercial echelle spectrographs. The lowest full width at half maximum of a peak achieved was 25 pm. The 2D spectrograph is based on the wavelength separation of light by the combination of a prism and a grating in one dimension, and an etalon in the second dimension. This instrument was successfully employed for the acquisition of Raman and laser-induced breakdown spectra.
Different spectroscopic methods (light scattering and fluorescence spectroscopy) permitting a spatial as well as spectral resolution, were used to investigate the release of ions in the electrospray. The investigation is based on the 50 nm shift of the fluorescence band of rhodamine 6G ions of during the transfer from the electrospray droplets to the gas phase.
A newly developed ionization chamber operating at reduced pressure (0.5 mbar) was coupled to a time-of-flight mass spectrometer. After REMPI of H2S, an ionization chemistry analogous to H2O was observed with this instrument. Besides H2S+ and its fragments, H3S+ and protonated analyte ions could be observed as a result of proton-transfer reactions.
For the elucidation of the peaks in IM spectra, a combination of IM spectrometer and linear quadrupole ion trap mass spectrometer was developed. The instrument can be equipped with various ionization sources (ESI, REMPI, APCI) and was used for the characterization of the peptide bradykinin and the neuroleptic promazine.
The ionization of explosive compounds in an APCI source based on soft x-radiation was investigated in a newly developed ionization chamber attached to the ion trap mass spectrometer. The major primary and secondary reactions could be characterized and explosive compound ions could be identified and assigned to the peaks in IM spectra. The assignment is based on the comparison of experimentally determined and calculated IM. The methods of calculation currently available exhibit large deviations, especially in the case of anions. Therefore, on the basis of an assessment of available methods, a novel hybrid method was developed and characterized.
We present new experimental data of the low-temperature metastable region of liquid water derived from high-density synthetic fluid inclusions (996–916 kg m−3) in quartz. Microthermometric measurements include: (i) prograde (upon heating) and retrograde (upon cooling) liquid–vapour homogenisation. We used single ultrashort laser pulses to stimulate vapour bubble nucleation in initially monophase liquid inclusions. Water densities were calculated based on prograde homogenisation temperatures using the IAPWS-95 formulation. We found retrograde liquid–vapour homogenisation temperatures in excellent agreement with IAPWS-95. (ii) Retrograde ice nucleation. Raman spectroscopy was used to determine the nucleation of ice in the absence of the vapour bubble. Our ice nucleation data in the doubly metastable region are inconsistent with the low-temperature trend of the spinodal predicted by IAPWS-95, as liquid water with a density of 921 kg m−3 remains in a homogeneous state during cooling down to a temperature of −30.5 °C, where it is transformed into ice whose density corresponds to zero pressure. (iii) Ice melting. Ice melting temperatures of up to 6.8 °C were measured in the absence of the vapour bubble, i.e. in the negative pressure region. (iv) Spontaneous retrograde and, for the first time, prograde vapour bubble nucleation. Prograde bubble nucleation occurred upon heating at temperatures above ice melting. The occurrence of prograde and retrograde vapour bubble nucleation in the same inclusions indicates a maximum of the bubble nucleation curve in the ϱ–T plane at around 40 °C. The new experimental data represent valuable benchmarks to evaluate and further improve theoretical models describing the p–V–T properties of metastable water in the low-temperature region.
Complexity in software systems is a major factor driving development and maintenance costs. To master this complexity, software is divided into modules that can be developed and tested separately. In order to support this separation of modules, each module should provide a clean and concise public interface. Therefore, the ability to selectively hide functionality using access control is an important feature in a programming language intended for complex software systems.
Software systems are increasingly distributed, adding not only to their inherent complexity, but also presenting security challenges. The object-capability approach addresses these challenges by defining language properties providing only minimal capabilities to objects. One programming language that is based on the object-capability approach is Newspeak, a dynamic programming language designed for modularity and security. The Newspeak specification describes access control as one of Newspeak’s properties, because it is a requirement for the object-capability approach. However, access control, as defined in the Newspeak specification, is currently not enforced in its implementation.
This work introduces an access control implementation for Newspeak, enabling the security of object-capabilities and enhancing modularity. We describe our implementation of access control for Newspeak. We adapted the runtime environment, the reflective system, the compiler toolchain, and the virtual machine. Finally, we describe a migration strategy for the existing Newspeak code base, so that our access control implementation can be integrated with minimal effort.
The Gradient Symbolic Computation (GSC) model presented in the keynote article (Goldrick, Putnam & Schwarz) constitutes a significant theoretical development, not only as a model of bilingual code-mixing, but also as a general framework that brings together symbolic grammars and graded representations. The authors are to be commended for successfully integrating a theory of grammatical knowledge with the voluminous research on lexical co-activation in bilinguals. It is, however, unfortunate that a certain conception of bilingualism was inherited from this latter research tradition, one in which the contrast between native and non-native language takes a back seat.
Eye movements serve as a window into ongoing visual-cognitive processes and can thus be used to investigate how people perceive real-world scenes. A key issue for understanding eye-movement control during scene viewing is the roles of central and peripheral vision, which process information differently and are therefore specialized for different tasks (object identification and peripheral target selection respectively). Yet, rather little is known about the contributions of central and peripheral processing to gaze control and how they are coordinated within a fixation during scene viewing. Additionally, the factors determining fixation durations have long been neglected, as scene perception research has mainly been focused on the factors determining fixation locations. The present thesis aimed at increasing the knowledge on how central and peripheral vision contribute to spatial and, in particular, to temporal aspects of eye-movement control during scene viewing. In a series of five experiments, we varied processing difficulty in the central or the peripheral visual field by attenuating selective parts of the spatial-frequency spectrum within these regions. Furthermore, we developed a computational model on how foveal and peripheral processing might be coordinated for the control of fixation duration. The thesis provides three main findings. First, the experiments indicate that increasing processing demands in central or peripheral vision do not necessarily prolong fixation durations; instead, stimulus-independent timing is adapted when processing becomes too difficult. Second, peripheral vision seems to play a prominent role in the control of fixation durations, a notion also implemented in the computational model. The model assumes that foveal and peripheral processing proceed largely in parallel and independently during fixation, but can interact to modulate fixation duration. Thus, we propose that the variation in fixation durations can in part be accounted for by the interaction between central and peripheral processing. Third, the experiments indicate that saccadic behavior largely adapts to processing demands, with a bias of avoiding spatial-frequency filtered scene regions as saccade targets. We demonstrate that the observed saccade amplitude patterns reflect corresponding modulations of visual attention. The present work highlights the individual contributions and the interplay of central and peripheral vision for gaze control during scene viewing, particularly for the control of fixation duration. Our results entail new implications for computational models and for experimental research on scene perception.
Optical biosensors based on porous silicon were fabricated by metal assisted chemical etching. Thereby double layered porous silicon structures were obtained consisting of porous pillars with large pores on top of a porous silicon layer with smaller pores. These structures showed a similar sensing performance in comparison to electrochemically produced porous silicon interferometric sensors.
Injection of fluids into deep saline aquifers causes a pore pressure increase in the storage formation, and thus displacement of resident brine. Via hydraulically conductive faults, brine may migrate upwards into shallower aquifers and lead to unwanted salinisation of potable groundwater resources. In the present study, we investigated different scenarios for a potential storage site in the Northeast German Basin using a three-dimensional (3-D) regional-scale model that includes four major fault zones. The focus was on assessing the impact of fault length and the effect of a secondary reservoir above the storage formation, as well as model boundary conditions and initial salinity distribution on the potential salinisation of shallow groundwater resources. We employed numerical simulations of brine injection as a representative fluid.
Our simulation results demonstrate that the lateral model boundary settings and the effective fault damage zone volume have the greatest influence on pressure build-up and development within the reservoir, and thus intensity and duration of fluid flow through the faults. Higher vertical pressure gradients for short fault segments or a small effective fault damage zone volume result in the highest salinisation potential due to a larger vertical fault height affected by fluid displacement. Consequently, it has a strong impact on the degree of shallow aquifer salinisation, whether a gradient in salinity exists or the saltwater-freshwater interface lies below the fluid displacement depth in the faults. A small effective fault damage zone volume or low fault permeability further extend the duration of fluid flow, which can persist for several tens to hundreds of years, if the reservoir is laterally confined. Laterally open reservoir boundaries, large effective fault damage zone volumes and intermediate reservoirs significantly reduce vertical brine migration and the potential of freshwater salinisation because the origin depth of displaced brine is located only a few decametres below the shallow aquifer in maximum.
The present study demonstrates that the existence of hydraulically conductive faults is not necessarily an exclusion criterion for potential injection sites, because salinisation of shallower aquifers strongly depends on initial salinity distribution, location of hydraulically conductive faults and their effective damage zone volumes as well as geological boundary conditions.
We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution.
Filling the Silence
(2016)
In a self-paced reading experiment, we investigated the processing of sluicing constructions (“sluices”) whose antecedent contained a known garden-path structure in German. Results showed decreased processing times for sluices with garden-path antecedents as well as a disadvantage for antecedents with non-canonical word order downstream from the ellipsis site. A post-hoc analysis showed the garden-path advantage also to be present in the region right before the ellipsis site. While no existing account of ellipsis processing explicitly predicted the results, we argue that they are best captured by combining a local antecedent mismatch effect with memory trace reactivation through reanalysis.
Many previous studies have shown that the turbulent mixing layer under periodic forcing tends to adopt a lock-on state, where the major portion of the fluctuations in the flow are synchronized at the forcing frequency. The goal of this experimental study is to apply closed-loop control in order to provoke the lock-on state, using information from the flow itself. We aim to determine the range of frequencies for which the closed-loop control can establish the lock-on, and what mechanisms are contributing to the selection of a feedback frequency. In order to expand the solution space for optimal closed-loop control laws, we use the genetic programming control (CPC) framework. The best closed-loop control laws obtained by CPC are analysed along with the associated physical mechanisms in the mixing layer flow. The resulting closed-loop control significantly outperforms open-loop forcing in terms of robustness to changes in the free-stream velocities. In addition, the selection of feedback frequencies is not locked to the most amplified local mode, but rather a range of frequencies around it.
Fruits exhibit a vast array of different 3D shapes, from simple spheres and cylinders to more complex curved forms; however, the mechanism by which growth is oriented and coordinated to generate this diversity of forms is unclear. Here, we compare the growth patterns and orientations for two very different fruit shapes in the Brassicaceae: the heart-shaped Capsella rubella silicle and the near-cylindrical Arabidopsis thaliana silique. We show, through a combination of clonal and morphological analyses, that the different shapes involve different patterns of anisotropic growth during three phases. These experimental data can be accounted for by a tissue level model in which specified growth rates vary in space and time and are oriented by a proximodistal polarity field. The resulting tissue conflicts lead to deformation of the tissue as it grows. The model allows us to identify tissue-specific and temporally specific activities required to obtain the individual shapes. One such activity may be provided by the valve-identity gene FRUITFULL, which we show through comparative mutant analysis to modulate fruit shape during post-fertilisation growth of both species. Simple modulations of the model presented here can also broadly account for the variety of shapes in other Brassicaceae species, thus providing a simplified framework for fruit development and shape diversity.