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Linked Open Data (LOD) comprises very many and often large public data sets and knowledge bases. Those datasets are mostly presented in the RDF triple structure of subject, predicate, and object, where each triple represents a statement or fact. Unfortunately, the heterogeneity of available open data requires significant integration steps before it can be used in applications. Meta information, such as ontological definitions and exact range definitions of predicates, are desirable and ideally provided by an ontology. However in the context of LOD, ontologies are often incomplete or simply not available. Thus, it is useful to automatically generate meta information, such as ontological dependencies, range definitions, and topical classifications. Association rule mining, which was originally applied for sales analysis on transactional databases, is a promising and novel technique to explore such data. We designed an adaptation of this technique for min-ing Rdf data and introduce the concept of “mining configurations”, which allows us to mine RDF data sets in various ways. Different configurations enable us to identify schema and value dependencies that in combination result in interesting use cases. To this end, we present rule-based approaches for auto-completion, data enrichment, ontology improvement, and query relaxation. Auto-completion remedies the problem of inconsistent ontology usage, providing an editing user with a sorted list of commonly used predicates. A combination of different configurations step extends this approach to create completely new facts for a knowledge base. We present two approaches for fact generation, a user-based approach where a user selects the entity to be amended with new facts and a data-driven approach where an algorithm discovers entities that have to be amended with missing facts. As knowledge bases constantly grow and evolve, another approach to improve the usage of RDF data is to improve existing ontologies. Here, we present an association rule based approach to reconcile ontology and data. Interlacing different mining configurations, we infer an algorithm to discover synonymously used predicates. Those predicates can be used to expand query results and to support users during query formulation. We provide a wide range of experiments on real world datasets for each use case. The experiments and evaluations show the added value of association rule mining for the integration and usability of RDF data and confirm the appropriateness of our mining configuration methodology.
This study investigates whether number dissimilarities on subject and object DPs facilitate the comprehension of subject-and object-extracted centre-embedded relative clauses in children with Grammatical Specific Language Impairment (G-SLI). We compared the performance of a group of English-speaking children with G-SLI (mean age: 12; 11) with that of two groups of younger typically developing (TD) children, matched on grammar and receptive vocabulary, respectively. All groups were more accurate on subject-extracted relative clauses than object-extracted ones and, crucially, they all showed greater accuracy for sentences with dissimilar number features (i.e., one singular, one plural) on the head noun and the embedded DP. These findings are interpreted in the light of current psycholinguistic models of sentence comprehension in TD children and provide further insight into the linguistic nature of G-SLI.
A dramatic efficiency improvement of bulk heterojunction solar cells based on electron-donating conjugated polymers in combination with soluble fullerene derivatives has been achieved over the past years. Certified and reported power conversion efficiencies now reach over 9% for single junctions and exceed the 10% benchmark for tandem solar cells. This trend brightens the vision of organic photovoltaics becoming competitive with inorganic solar cells including the realization of low-cost and large-area organic photovoltaics. For the best performing organic materials systems, the yield of charge generation can be very efficient. However, a detailed understanding of the free charge carrier generation mechanisms at the donor acceptor interface and the energy loss associated with it needs to be established. Moreover, organic solar cells are limited by the competition between charge extraction and free charge recombination, accounting for further efficiency losses. A conclusive picture and the development of precise methodologies for investigating the fundamental processes in organic solar cells are crucial for future material design, efficiency optimization, and the implementation of organic solar cells into commercial products.
In order to advance the development of organic photovoltaics, my thesis focuses on the comprehensive understanding of charge generation, recombination and extraction in organic bulk heterojunction solar cells summarized in 6 chapters on the cumulative basis of 7 individual publications.
The general motivation guiding this work was the realization of an efficient hybrid inorganic/organic tandem solar cell with sub-cells made from amorphous hydrogenated silicon and organic bulk heterojunctions. To realize this project aim, the focus was directed to the low band-gap copolymer PCPDTBT and its derivatives, resulting in the examination of the charge carrier dynamics in PCPDTBT:PC70BM blends in relation to by the blend morphology. The phase separation in this blend can be controlled by the processing additive diiodooctane, enhancing domain purity and size. The quantitative investigation of the free charge formation was realized by utilizing and improving the time delayed collection field technique. Interestingly, a pronounced field dependence of the free carrier generation for all blends is found, with the field dependence being stronger without the additive. Also, the bimolecular recombination coefficient for both blends is rather high and increases with decreasing internal field which we suggest to be caused by a negative field dependence of mobility. The additive speeds up charge extraction which is rationalized by the threefold increase in mobility.
By fluorine attachment within the electron deficient subunit of PCPDTBT, a new polymer F-PCPDTBT is designed. This new material is characterized by a stronger tendency to aggregate as compared to non-fluorinated PCPDTBT. Our measurements show that for F-PCPDTBT:PCBM blends the charge carrier generation becomes more efficient and the field-dependence of free charge carrier generation is weakened. The stronger tendency to aggregate induced by the fluorination also leads to increased polymer rich domains, accompanied in a threefold reduction in the non-geminate recombination coefficient at conditions of open circuit. The size of the polymer domains is nicely correlated to the field-dependence of charge generation and the Langevin reduction factor, which highlights the importance of the domain size and domain purity for efficient charge carrier generation. In total, fluorination of PCPDTBT causes the PCE to increase from 3.6 to 6.1% due to enhanced fill factor, short circuit current and open circuit voltage. Further optimization of the blend ratio, active layer thickness, and polymer molecular weight resulted in 6.6% efficiency for F-PCPDTBT:PC70BM solar cells.
Interestingly, the double fluorinated version 2F-PCPDTBT exhibited poorer FF despite a further reduction of geminate and non-geminate recombination losses. To further analyze this finding, a new technique is developed that measures the effective extraction mobility under charge carrier densities and electrical fields comparable to solar cell operation conditions. This method involves the bias enhanced charge extraction technique. With the knowledge of the carrier density under different electrical field and illumination conditions, a conclusive picture of the changes in charge carrier dynamics leading to differences in the fill factor upon fluorination of PCPDTBT is attained. The more efficient charge generation and reduced recombination with fluorination is counterbalanced by a decreased extraction mobility. Thus, the highest fill factor of 60% and efficiency of 6.6% is reached for F-PCPDTBT blends, while 2F-PCPDTBT blends have only moderate fill factors of 54% caused by the lower effective extraction mobility, limiting the efficiency to 6.5%.
To understand the details of the charge generation mechanism and the related losses, we evaluated the yield and field-dependence of free charge generation using time delayed collection field in combination with sensitive measurements of the external quantum efficiency and absorption coefficients for a variety of blends. Importantly, both the yield and field-dependence of free charge generation is found to be unaffected by excitation energy, including direct charge transfer excitation below the optical band gap. To access the non-detectable absorption at energies of the relaxed charge transfer emission, the absorption was reconstructed from the CT emission, induced via the recombination of thermalized charges in electroluminescence. For a variety of blends, the quantum yield at energies of charge transfer emission was identical to excitations with energies well above the optical band-gap. Thus, the generation proceeds via the split-up of the thermalized charge transfer states in working solar cells. Further measurements were conducted on blends with fine-tuned energy levels and similar blend morphologies by using different fullerene derivatives. A direct correlation between the efficiency of free carrier generation and the energy difference of the relaxed charge transfer state relative to the energy of the charge separated state is found. These findings open up new guidelines for future material design as new high efficiency materials require a minimum energetic offset between charge transfer and the charge separated state while keeping the HOMO level (and LUMO level) difference between donor and acceptor as small as possible.
This reference paper describes the sampling and contents of the IZA Evaluation Dataset Survey and outlines its vast potential for research in labor economics. The data have been part of a unique IZA project to connect administrative data from the German Federal Employment Agency with innovative survey data to study the out-mobility of individuals to work. This study makes the survey available to the research community as a Scientific Use File by explaining the development, structure, and access to the data. Furthermore, it also summarizes previous findings with the survey data.
Adopting a minimalist framework, the dissertation provides an analysis for the syntactic structure of comparatives, with special attention paid to the derivation of the subclause. The proposed account explains how the comparative subclause is connected to the matrix clause, how the subclause is formed in the syntax and what additional processes contribute to its final structure. In addition, it casts light upon these problems in cross-linguistic terms and provides a model that allows for synchronic and diachronic differences. This also enables one to give a more adequate explanation for the phenomena found in English comparatives since the properties of English structures can then be linked to general settings of the language and hence need no longer be considered as idiosyncratic features of the grammar of English. First, the dissertation provides a unified analysis of degree expressions, relating the structure of comparatives to that of other degrees. It is shown that gradable adjectives are located within a degree phrase (DegP), which in turn projects a quantifier phrase (QP) and that these two functional layers are always present, irrespectively of whether there is a phonologically visible element in these layers. Second, the dissertation presents a novel analysis of Comparative Deletion by reducing it to an overtness constraint holding on operators: in this way, it is reduced to morphological differences and cross-linguistic variation is not conditioned by way of postulating an arbitrary parameter. Cross-linguistic differences are ultimately dependent on whether a language has overt operators equipped with the relevant – [+compr] and [+rel] – features. Third, the dissertation provides an adequate explanation for the phenomenon of Attributive Comparative Deletion, as attested in English, by way of relating it to the regular mechanism of Comparative Deletion. I assume that Attributive Comparative Deletion is not a universal phenomenon, and its presence in English can be conditioned by independent, more general rules, while the absence of such restrictions leads to its absence in other languages. Fourth, the dissertation accounts for certain phenomena related to diachronic changes, examining how the changes in the status of comparative operators led to changes in whether Comparative Deletion is attested in a given language: I argue that only operators without a lexical XP can be grammaticalised. The underlying mechanisms underlying are essentially general economy principles and hence the processes are not language-specific or exceptional. Fifth, the dissertation accounts for optional ellipsis processes that play a crucial role in the derivation of typical comparative subclauses. These processes are not directly related to the structure of degree expressions and hence the elimination of the quantified expression from the subclause; nevertheless, they are shown to be in interaction with the mechanisms underlying Comparative Deletion or the absence thereof.
Biosensors for the detection of benzaldehyde and g-aminobutyric acid (GABA) are reported using aldehyde oxidoreductase PaoABC from Escherichia coli immobilized in a polymer containing bound low potential osmium redox complexes. The electrically connected enzyme already electrooxidizes benzaldehyde at potentials below −0.15 V (vs. Ag|AgCl, 1 M KCl). The pH-dependence of benzaldehyde oxidation can be strongly influenced by the ionic strength. The effect is similar with the soluble osmium redox complex and therefore indicates a clear electrostatic effect on the bioelectrocatalytic efficiency of PaoABC in the osmium containing redox polymer. At lower ionic strength, the pH-optimum is high and can be switched to low pH-values at high ionic strength. This offers biosensing at high and low pH-values. A “reagentless” biosensor has been formed with enzyme wired onto a screen-printed electrode in a flow cell device. The response time to addition of benzaldehyde is 30 s, and the measuring range is between 10–150 µM and the detection limit of 5 µM (signal to noise ratio 3:1) of benzaldehyde. The relative standard deviation in a series (n = 13) for 200 µM benzaldehyde is 1.9%. For the biosensor, a response to succinic semialdehyde was also identified. Based on this response and the ability to work at high pH a biosensor for GABA is proposed by coimmobilizing GABA-aminotransferase (GABA-T) and PaoABC in the osmium containing redox polymer.
DNA origami nanostructures allow for the arrangement of different functionalities such as proteins, specific DNA structures, nanoparticles, and various chemical modifications with unprecedented precision. The arranged functional entities can be visualized by atomic force microscopy (AFM) which enables the study of molecular processes at a single-molecular level. Examples comprise the investigation of chemical reactions, electron-induced bond breaking, enzymatic binding and cleavage events, and conformational transitions in DNA. In this paper, we provide an overview of the advances achieved in the field of single-molecule investigations by applying atomic force microscopy to functionalized DNA origami substrates.
On the role of fluoro-substituted nucleosides in DNA radiosensitization for tumor radiation therapy
(2014)
Gemcitabine (2′,2′-difluorocytidine) is a well-known radiosensitizer routinely applied in concomitant chemoradiotherapy. During irradiation of biological media with high-energy radiation secondary low-energy (<10 eV) electrons are produced that can directly induce chemical bond breakage in DNA by dissociative electron attachment (DEA). Here, we investigate and compare DEA to the three molecules 2′-deoxycytidine, 2′-deoxy-5-fluorocytidine, and gemcitabine. Fluorination at specific molecular sites, i.e., nucleobase or sugar moiety, is found to control electron attachment and subsequent dissociation pathways. The presence of two fluorine atoms at the sugar ring results in more efficient electron attachment to the sugar moiety and subsequent bond cleavage. For the formation of the dehydrogenated nucleobase anion, we obtain an enhancement factor of 2.8 upon fluorination of the sugar, whereas the enhancement factor is 5.5 when the nucleobase is fluorinated. The observed fragmentation reactions suggest enhanced DNA strand breakage induced by secondary electrons when gemcitabine is incorporated into DNA.