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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.