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The Tibetan Plateau is the largest elevated landmass in the world and profoundly influences atmospheric circulation patterns such as the Asian monsoon system. Therefore this area has been increasingly in focus of palaeoenvironmental studies. This thesis evaluates the applicability of organic biomarkers for palaeolimnological purposes on the Tibetan Plateau with a focus on aquatic macrophyte-derived biomarkers. Submerged aquatic macrophytes have to be considered to significantly influence the sediment organic matter due to their high abundance in many Tibetan lakes. They can show highly 13C-enriched biomass because of their carbon metabolism and it is therefore crucial for the interpretation of δ13C values in sediment cores to understand to which extent aquatic macrophytes contribute to the isotopic signal of the sediments in Tibetan lakes and in which way variations can be explained in a palaeolimnological context. Additionally, the high abundance of macrophytes makes them interesting as potential recorders of lake water δD. Hydrogen isotope analysis of biomarkers is a rapidly evolving field to reconstruct past hydrological conditions and therefore of special relevance on the Tibetan Plateau due to the direct linkage between variations of monsoon intensity and changes in regional precipitation / evaporation balances. A set of surface sediment and aquatic macrophyte samples from the central and eastern Tibetan Plateau was analysed for composition as well as carbon and hydrogen isotopes of n-alkanes. It was shown how variable δ13C values of bulk organic matter and leaf lipids can be in submerged macrophytes even of a single species and how strongly these parameters are affected by them in corresponding sediments. The estimated contribution of the macrophytes by means of a binary isotopic model was calculated to be up to 60% (mean: 40%) to total organic carbon and up to 100% (mean: 66%) to mid-chain n-alkanes. Hydrogen isotopes of n-alkanes turned out to record δD of meteoric water of the summer precipitation. The apparent enrichment factor between water and n-alkanes was in range of previously reported ones (≈-130‰) at the most humid sites, but smaller (average: -86‰) at sites with a negative moisture budget. This indicates an influence of evaporation and evapotranspiration on δD of source water for aquatic and terrestrial plants. The offset between δD of mid- and long-chain n-alkanes was close to zero in most of the samples, suggesting that lake water as well as soil and leaf water are affected to a similar extent by those effects. To apply biomarkers in a palaeolimnological context, the aliphatic biomarker fraction of a sediment core from Lake Koucha (34.0° N; 97.2° E; eastern Tibetan Plateau) was analysed for concentrations, δ13C and δD values of compounds. Before ca. 8 cal ka BP, the lake was dominated by aquatic macrophyte-derived mid-chain n-alkanes, while after 6 cal ka BP high concentrations of a C20 highly branched isoprenoid compound indicate a predominance of phytoplankton. Those two principally different states of the lake were linked by a transition period with high abundances of microbial biomarkers. δ13C values were relatively constant for long-chain n-alkanes, while mid-chain n-alkanes showed variations between -23.5 to -12.6‰. Highest values were observed for the assumed period of maximum macrophyte growth during the late glacial and for the phytoplankton maximum during the middle and late Holocene. Therefore, the enriched values were interpreted to be caused by carbon limitation which in turn was induced by high macrophyte and primary productivity, respectively. Hydrogen isotope signatures of mid-chain n-alkanes have been shown to be able to track a previously deduced episode of reduced moisture availability between ca. 10 and 7 cal ka BP, indicated by a 20‰ shift towards higher δD values. Indications for cooler episodes at 6.0, 3.1 and 1.8 cal ka BP were gained from drops of biomarker concentrations, especially microbial-derived hopanoids, and from coincidental shifts towards lower δ13C values. Those episodes correspond well with cool events reported from other locations on the Tibetan Plateau as well as in the Northern Hemisphere. To conclude, the study of recent sediments and plants improved the understanding of factors affecting the composition and isotopic signatures of aliphatic biomarkers in sediments. Concentrations and isotopic signatures of the biomarkers in Lake Koucha could be interpreted in a palaeolimnological context and contribute to the knowledge about the history of the lake. Aquatic macrophyte-derived mid-chain n-alkanes were especially useful, due to their high abundance in many Tibetan Lakes and their ability to record major changes of lake productivity and palaeo-hydrological conditions. Therefore, they have the potential to contribute to a fuller understanding of past climate variability in this key region for atmospheric circulation systems.
Many formal descriptions of DPLL-based SAT algorithms either do not include all essential proof techniques applied by modern SAT solvers or are bound to particular heuristics or data structures. This makes it difficult to analyze proof-theoretic properties or the search complexity of these algorithms. In this paper we try to improve this situation by developing a nondeterministic proof calculus that models the functioning of SAT algorithms based on the DPLL calculus with clause learning. This calculus is independent of implementation details yet precise enough to enable a formal analysis of realistic DPLL-based SAT algorithms.
We study buckling instabilities of filaments in biological systems. Filaments in a cell are the building blocks of the cytoskeleton. They are responsible for the mechanical stability of cells and play an important role in intracellular transport by molecular motors, which transport cargo such as organelles along cytoskeletal filaments. Filaments of the cytoskeleton are semiflexible polymers, i.e., their bending energy is comparable to the thermal energy such that they can be viewed as elastic rods on the nanometer scale, which exhibit pronounced thermal fluctuations. Like macroscopic elastic rods, filaments can undergo a mechanical buckling instability under a compressive load. In the first part of the thesis, we study how this buckling instability is affected by the pronounced thermal fluctuations of the filaments. In cells, compressive loads on filaments can be generated by molecular motors. This happens, for example, during cell division in the mitotic spindle. In the second part of the thesis, we investigate how the stochastic nature of such motor-generated forces influences the buckling behavior of filaments. In chapter 2 we review briefly the buckling instability problem of rods on the macroscopic scale and introduce an analytical model for buckling of filaments or elastic rods in two spatial dimensions in the presence of thermal fluctuations. We present an analytical treatment of the buckling instability in the presence of thermal fluctuations based on a renormalization-like procedure in terms of the non-linear sigma model where we integrate out short-wavelength fluctuations in order to obtain an effective theory for the mode of the longest wavelength governing the buckling instability. We calculate the resulting shift of the critical force by fluctuation effects and find that, in two spatial dimensions, thermal fluctuations increase this force. Furthermore, in the buckled state, thermal fluctuations lead to an increase in the mean projected length of the filament in the force direction. As a function of the contour length, the mean projected length exhibits a cusp at the buckling instability, which becomes rounded by thermal fluctuations. Our main result is the observation that a buckled filament is stretched by thermal fluctuations, i.e., its mean projected length in the direction of the applied force increases by thermal fluctuations. Our analytical results are confirmed by Monte Carlo simulations for buckling of semiflexible filaments in two spatial dimensions. We also perform Monte Carlo simulations in higher spatial dimensions and show that the increase in projected length by thermal fluctuations is less pronounced than in two dimensions and strongly depends on the choice of the boundary conditions. In the second part of this work, we present a model for buckling of semiflexible filaments under the action of molecular motors. We investigate a system in which a group of motors moves along a clamped filament carrying a second filament as a cargo. The cargo-filament is pushed against the wall and eventually buckles. The force-generating motors can stochastically unbind and rebind to the filament during the buckling process. We formulate a stochastic model of this system and calculate the mean first passage time for the unbinding of all linking motors which corresponds to the transition back to the unbuckled state of the cargo filament in a mean-field model. Our results show that for sufficiently short microtubules the movement of kinesin-I-motors is affected by the load force generated by the cargo filament. Our predictions could be tested in future experiments.
The acquisition of phonological alternations consists of many aspects as discussions in the relevant literature show. There are contrary findings about the role of naturalness. A natural process is grounded in phonetics; they are easy to learn, even in second language acquisition when adults have to learn certain processes that do not occur in their native language. There is also evidence that unnatural – arbitrary – rules can be learned. Current work on the acquisition of morphophonemic alternations suggests that their probability of occurrence is a crucial factor in acquisition. I have conducted an experiment to investigate the effects of naturalness as well as of probability of occurrence with 80 adult native speakers of German. It uses the Artificial Grammar paradigm: Two artificial languages were constructed, each with a particular alternation. In one language the alternation is natural (vowel harmony); in the other language the alternation is arbitrary (a vowel alternation depends on the sonorancy of the first consonant of the stem). The participants were divided in two groups, one group listened to the natural alternation and the other group listened to the unnatural alternation. Each group was divided into two subgroups. One subgroup then was presented with material in which the alternation occurred frequently and the other subgroup was presented with material in which the alternation occurred infrequently. After this exposure phase every participant was asked to produce new words during the test phase. Knowledge about the language-specific alternation pattern was needed to produce the forms correctly as the phonological contexts demanded certain alternants. The group performances have been compared with respect to the effects of naturalness and probability of occurrence. The natural rule was learned more easily than the unnatural one. Frequently presented rules were not learned more easily than the ones that were presented less frequently. Moreover, participants did not learn the unnatural rule at all, whether this rule was presented frequently or infrequently did not matter. There was a tendency that the natural rule was learned more easily if presented frequently than if presented infrequently, but it was not significant due to variability across participants.
Foreland-basin systems are excellent archives to decipher the feedbacks between surface and tectonic processes in orogens. The sedimentary architecture of a foreland-basin system reflects the balance between tectonic subsidence causing long-term accommodation space and sediment influx corresponding to efficiency of erosion and mass-redistribution processes. In order to explore the effects of climatic and tectonic forcing in such a system, I investigated the Oligo-Miocene foreland-basin sediments of the southern Alborz mountains, an intracontinental orogen in northern Iran, related to the Arabia-Eurasia continental collision. This work includes absolute dating methods such as 40Ar/39Ar and zircon (U-Th)/He thermochronology, magnetostratigraphy, sedimentological analysis, sandstone and conglomerate provenance study, carbon and oxygen isotope analysis, and clay mineralogy study. Results show a systematic correlation between coarsening-upward cycles and sediment accumulation rates in the basin on 105 to 106yr time scales. During thrust loading phases, the coarse-grained fraction supplied by the uplifting range is stored in the proximal part of the basin (sedimentary facies retrogradation), while fine-grained sediments are deposited in distal sectors. Variations in sediment provenance during these phases of enhanced tectonic activity give evidence for erosional unroofing phases and/or drainage-reorganization events. In addition, enhanced tectonic activity promoted the growth of topography and associated orographic barrier effects, as demonstrated by sedimentologic indicators and the analysis of stable C and O isotopes from calcareous paleosols and lacustrine/palustrine samples. Extensive progradation of coarse-grained deposits occurs during phases of decreased subsidence, when the coarse-grained fraction supplied by the uplifting range cannot be completely stored in the proximal part of the basin. In this environment, a reduction in basin subsidence is associated with laterally stacked fluvial channel deposits, and is related to intra-foreland uplift, as documented by growth strata, tectonic tilting, and sediment reworking. Increase in sediment accumulation rate associated with progradation of vertically-stacked coarse-grained fluvial channels also occurs. Paleosol O-isotope data shows that this increase is related to wetter climatic phases, suggesting that surface processes are more efficient and exhumation rates increase, giving rise to a positive feedback. Furthermore, isotopic and sedimentologic data show that starting from 10-9 Ma, climate became less arid with an increase in seasonality of precipitation. Because important changes were also recorded in the Mediterranean Sea and Asia at that time, the evidence for climatic variability observed in the Alborz mountains most likely reflects changes in Northern Hemisphere atmospheric circulation patterns. This study has additional implications for the evolution of the Alborz mountains and the Arabia-Eurasia continental collision zone. At the orogenic scale, the locus of deformation did not move steadily southward, but stepped forward and backward since Oligocene time. In particular, from ~ 17.5 to 6.2 Ma the orogen grew by a combination of frontal accretion and wedge-internal deformation on time scales of ca. 0.7 to 2 m.y. Moreover, the provenance data suggest that prior to 10-9 Ma the shortening direction changed from NW-SE to NNE-SSW, in agreement with structural data. On the scale of the entire collision zone, the evolution of the studied basins and adjacent mountain ranges suggests a new geodynamic model for the evolution of the Arabia-Eurasia continental collision zone. Numerous sedimentary basins in the Alborz mountains and in other locations of the Arabia-Eurasia collision zone record a change from a tensional (transtensional) to a compressional (transpressional) tectonic setting by ~ 36 Ma. I interpret this to reflect the onset of subduction of the stretched Arabian continental lithosphere beneath central Iran, leading to moderate plate coupling and lower- and upper-plate deformation (soft continental collision). The increase in deformation rates in the southern Alborz mountains from ~ 17.5 Ma suggests that significant upper-plate deformation must have started by the early Miocene most likely in response to an increase in degree of plate coupling. I suggest that this was related to the subduction of thicker Arabian continental lithosphere and the consequent onset of hard continental collision. This model reconciles the apparent lag time of 15-20 m.y between the late Eocene to early Oligocene age for the initial Arabia-Eurasia continental collision and the onset of widespread deformation across the collision zone to the north in early to late Miocene time.
Classical semiconductor physics has been continuously improving electronic components such as diodes, light-emitting diodes, solar cells and transistors based on highly purified inorganic crystals over the past decades. Organic semiconductors, notably polymeric, are a comparatively young field of research, the first light-emitting diode based on conjugated polymers having been demonstrated in 1990. Polymeric semiconductors are of tremendous interest for high-volume, low-cost manufacturing ("printed electronics"). Due to their rather simple device structure mostly comprising only one or two functional layers, polymeric diodes are much more difficult to optimize compared to small-molecular organic devices. Usually, functions such as charge injection and transport are handled by the same material which thus needs to be highly optimized. The present work contributes to expanding the knowledge on the physical mechanisms determining device performance by analyzing the role of charge injection and transport on device efficiency for blue and white-emitting devices, based on commercially relevant spiro-linked polyfluorene derivatives. It is shown that such polymers can act as very efficient electron conductors and that interface effects such as charge trapping play the key role in determining the overall device efficiency. This work contributes to the knowledge of how charges drift through the polymer layer to finally find neutral emissive trap states and thus allows a quantitative prediction of the emission color of multichromophoric systems, compatible with the observed color shifts upon driving voltage and temperature variation as well as with electrical conditioning effects. In a more methodically oriented part, it is demonstrated that the transient device emission observed upon terminating the driving voltage can be used to monitor the decay of geminately-bound species as well as to determine trapped charge densities. This enables direct comparisons with numerical simulations based on the known properties of charge injection, transport and recombination. The method of charge extraction under linear increasing voltages (CELIV) is investigated in some detail, correcting for errors in the published approach and highlighting the role of non-idealized conditions typically present in experiments. An improved method is suggested to determine the field dependence of charge mobility in a more accurate way. Finally, it is shown that the neglect of charge recombination has led to a misunderstanding of experimental results in terms of a time-dependent mobility relaxation.
Service-oriented modeling employs collaborations to capture the coordination of multiple roles in form of service contracts. In case of dynamic collaborations the roles may join and leave the collaboration at runtime and therefore complex structural dynamics can result, which makes it very hard to ensure their correct and safe operation. We present in this paper our approach for modeling and verifying such dynamic collaborations. Modeling is supported using a well-defined subset of UML class diagrams, behavioral rules for the structural dynamics, and UML state machines for the role behavior. To be also able to verify the resulting service-oriented systems, we extended our former results for the automated verification of systems with structural dynamics [7, 8] and developed a compositional reasoning scheme, which enables the reuse of verification results. We outline our approach using the example of autonomous vehicles that use such dynamic collaborations via ad-hoc networking to coordinate and optimize their joint behavior.
This work presents the synthesis and the self-assembly of symmetrical amphiphilic ABA and BAB triblock copolymers in dilute, semi-concentrated and highly concentrated aqueous solution. A series of new bifunctional bistrithiocarbonates as RAFT agents was used to synthesise these triblock copolymers, which are characterised by a long hydrophilic middle block and relatively small, but strongly hydrophobic end blocks. As hydrophilic A blocks, poly(N-isopropylacrylamide) (PNIPAM) and poly(methoxy diethylene glycol acrylate) (PMDEGA) were employed, while as hydrophobic B blocks, poly(4-tert-butyl styrene), polystyrene, poly(3,5-dibromo benzyl acrylate), poly(2-ethylhexyl acrylate), and poly(octadecyl acrylate) were explored as building blocks with different hydrophobicities and glass transition temperatures. The five bifunctional trithiocarbonates synthesised belong to two classes: the first are RAFT agents, which position the active group of the growing polymer chain at the outer ends of the polymer (Z-C(=S)-S-R-S-C(=S)-Z, type I). The second class places the active groups in the middle of the growing polymer chain (R-S-C(=S)-Z-C(=S)-S-R, type II). These RAFT agents enable the straightforward synthesis of amphiphilic triblock copolymers in only two steps, allowing to vary the nature of the hydrophobic blocks as well as the length of the hydrophobic and hydrophilic blocks broadly with good molar mass control and narrow polydispersities. Specific side reactions were observed among some RAFT agents including the elimination of ethylenetrithiocarbonate in the early stage of the polymerisation of styrene mediated by certain agents of the type II, while the use of the RAFT agents of type I resulted in retardation of the chain extension of PNIPAM with styrene. These results underline the need of a careful choice of RAFT agents for a given task. The various copolymers self-assemble in dilute and semi-concentrated aqueous solution into small flower-like micelles. No indication for the formation of micellar clusters was found, while only at high concentration, physical hydrogels are formed. The reversible thermoresponsive behaviour of the ABA and BAB type copolymer solutions in water with A made of PNIPAM was examined by turbidimetry and dynamic light scattering (DLS). The cloud point of the copolymers was nearly identical to the cloud point of the homopolymer and varied between 28-32 °C with concentrations from 0.01 to 50 wt%. This is attributed to the formation of micelles where the hydrophobic blocks are shielded from a direct contact with water, so that the hydrophobic interactions of the copolymers are nearly the same as for pure PNIPAM. Dynamic light scattering measurements showed the presence of small micelles at ambient temperature. The aggregate size dramatically increased above the cloud point, indicating a change of aggregate morphology into clusters due to the thermosensitivity of the PNIPAM block. The rheological behaviour of the amphiphilic BAB triblock copolymers demonstrated the formation of hydrogels at high concentrations, typically above 30-35 wt%. The minimum concentration to induce hydrogels decreased with the increasing glass transition temperatures and increasing length of the end blocks. The weak tendency to form hydrogels was attributed to a small share of bridged micelles only, due to the strong segregation regime occurring. In order to learn about the role of the nature of the thermoresponsive block for the aggregation, a new BAB triblock copolymer consisting of short polystyrene end blocks and PMDEGA as stimuli-responsive middle block was prepared and investigated. Contrary to PNIPAM, dilute aqueous solutions of PMDEGA and of its block copolymers showed reversible phase transition temperatures characterised by a strong dependence on the polymer composition. Moreover, the PMDEGA block copolymer allowed the formation of physical hydrogels at lower concentration, i.e. from 20 wt%. This result suggests that PMDEGA has a higher degree of water-swellability than PNIPAM.
‘Heterosis’ is a term used in genetics and breeding referring to hybrid vigour or the superiority of hybrids over their parents in terms of traits such as size, growth rate, biomass, fertility, yield, nutrient content, disease resistance or tolerance to abiotic and abiotic stress. Parental plants which are two different inbred (pure) lines that have desired traits are crossed to obtain hybrids. Maximum heterosis is observed in the first generation (F1) of crosses. Heterosis has been utilised in plant and animal breeding programs for at least 90 years: by the end of the 21st century, 65% of worldwide maize production was hybrid-based. Generally, it is believed that an understanding of the molecular basis of heterosis will allow the creation of new superior genotypes which could either be used directly as F1 hybrids or form the basis for the future breeding selection programmes. Two selected accessions of a research model plant Arabidopsis thaliana (thale cress) were crossed to obtain hybrids. These typically exhibited a 60-80% increase of biomass when compared to the average weight of both parents. This PhD project focused on investigating the role of selected regulatory genes given their potentially key involvement in heterosis. In the first part of the project, the most appropriate developmental stage for this heterosis study was determined by metabolite level measurements and growth observations in parents and hybrids. At the selected stage, around 60 candidate regulatory genes (i.e. differentially expressed in hybrids when compared to parents) were identified. Of these, the majority were transcription factors, genes that coordinate the expression of other genes. Subsequent expression analyses of the candidate genes in biomass-heterotic hybrids of other Arabidopsis accessions revealed a differential expression in a gene subset, highlighting their relevance for heterosis. Moreover, a fraction of the candidate regulatory genes were found within DNA regions closely linked to the genes that underlie the biomass or growth heterosis. Additional analyses to validate the role of selected candidate regulatory genes in heterosis appeared insufficient to establish their role in heterosis. This uncovered a need for using novel approaches as discussed in the thesis. Taken together, the work provided an insight into studies on the molecular mechanisms underlying heterosis. Although studies on heterosis date back to more than one hundred years, this project as many others revealed that more investigations will be needed to uncover this phenomenon.
Background: Phylogenomic analyses recently became popular to address questions about deep metazoan phylogeny. Ribosomal proteins (RP) dominate many of these analyses or are, in some cases, the only genes included. Despite initial hopes, hylogenomic analyses including tens to hundreds of genes still fail to robustly place many bilaterian taxa. Results: Using the phylogenetic position of myzostomids as an example, we show that phylogenies derived from RP genes and mitochondrial genes produce incongruent results. Whereas the former support a position within a clade of platyzoan taxa, mitochondrial data recovers an annelid affinity, which is strongly supported by the gene order data and is congruent with morphology. Using hypothesis testing, our RP data significantly rejects the annelids affinity, whereas a platyzoan relationship is significantly rejected by the mitochondrial data. Conclusion: We conclude (i) that reliance of a set of markers belonging to a single class of macromolecular complexes might bias the analysis, and (ii) that concatenation of all available data might introduce conflicting signal into phylogenetic analyses. We therefore strongly recommend testing for data incongruence in phylogenomic analyses. Furthermore, judging all available data, we consider the annelid affinity hypothesis more plausible than a possible platyzoan affinity for myzostomids, and suspect long branch attraction is influencing the RP data. However, this hypothesis needs further confirmation by future analyses.
The phenolamines octopamine and tyramine control, regulate, and modulate many physiological and behavioral processes in invertebrates. Vertebrates possess only small amounts of both substances, and thus, octopamine and tyramine, together with other biogenic amines, are referred to as “trace amines.” Biogenic amines evoke cellular responses by activating G-protein-coupled receptors. We have isolated a complementary DNA (cDNA) that encodes a biogenic amine receptor from the American cockroach Periplaneta americana, viz., Peatyr1, which shares high sequence similarity to members of the invertebrate tyramine-receptor family. The PeaTYR1 receptor was stably expressed in human embryonic kidney (HEK) 293 cells, and its ligand response has been examined. Receptor activation with tyramine reduces adenylyl cyclase activity in a dose-dependent manner (EC50 350 nM). The inhibitory effect of tyramine is abolished by co-incubation with either yohimbine or chlorpromazine. Receptor expression has been investigated by reverse transcription polymerase chain reaction and immunocytochemistry. The mRNA is present in various tissues including brain, salivary glands, midgut, Malpighian tubules, and leg muscles. The effect of tyramine on salivary gland acinar cells has been investigated by intracellular recordings, which have revealed excitatory presynaptic actions of tyramine. This study marks the first comprehensive molecular, pharmacological, and functional characterization of a tyramine receptor in the cockroach.
Source, topography and excitatory effects of GABAergic innervation in cockroach salivary glands
(2009)
Cockroach salivary glands are innervated by dopaminergic and serotonergic neurons. Both transmitters elicit saliva secretion. We studied the distribution pattern of neurons containing gamma-aminobutyric acid ( GABA) and their physiological role. Immunofluorescence revealed a GABA-immunoreactive axon that originates within the subesophageal ganglion at the salivary neuron 2 (SN2) and this extends within the salivary duct nerve towards the salivary gland. GABA-positive fibers form a network on most acinar lobules and a dense plexus in the interior of a minor fraction of acinar lobules. Co-staining with anti-synapsin revealed that some putative GABAergic terminals seem to make pre-synaptic contacts with GABA-negative release sites. Many putative GABAergic release sites are at some distance from other synapses and at distance from the acinar tissue. Intracellular recordings from isolated salivary glands have revealed that GABA does not affect the basolateral membrane potential of the acinar cells directly. When applied during salivary duct nerve stimulation, GABA enhances the electrical response of the acinar cells and increases the rates of fluid and protein secretion. The effect on electrical cell responses is mimicked by the GABA(B) receptor agonists baclofen and SKF97541, and blocked by the GABAB receptor antagonists CGP52432 and CGP54626. These findings indicate that GABA has a modulatory role in the control of salivation, acting presynaptically on serotonergic and/or dopaminergic neurotransmission.
Spatial patterns as well as temporal dynamics of soil moisture have a major influence on runoff generation. The investigation of these dynamics and patterns can thus yield valuable information on hydrological processes, especially in data scarce or previously ungauged catchments. The combination of spatially scarce but temporally high resolution soil moisture profiles with episodic and thus temporally scarce moisture profiles at additional locations provides information on spatial as well as temporal patterns of soil moisture at the hillslope transect scale. This approach is better suited to difficult terrain (dense forest, steep slopes) than geophysical techniques and at the same time less cost-intensive than a high resolution grid of continuously measuring sensors. Rainfall simulation experiments with dye tracers while continuously monitoring soil moisture response allows for visualization of flow processes in the unsaturated zone at these locations. Data was analyzed at different spacio-temporal scales using various graphical methods, such as space-time colour maps (for the event and plot scale) and binary indicator maps (for the long-term and hillslope scale). Annual dynamics of soil moisture and decimeterscale variability were also investigated. The proposed approach proved to be successful in the investigation of flow processes in the unsaturated zone and showed the importance of preferential flow in the Malalcahuello Catchment, a datascarce catchment in the Andes of Southern Chile. Fast response times of stream flow indicate that preferential flow observed at the plot scale might also be of importance at the hillslope or catchment scale. Flow patterns were highly variable in space but persistent in time. The most likely explanation for preferential flow in this catchment is a combination of hydrophobicity, small scale heterogeneity in rainfall due to redistribution in the canopy and strong gradients in unsaturated conductivities leading to self-reinforcing flow paths.
In the first section of the thesis graphitic carbon nitride was for the first time synthesised using the high-temperature condensation of dicyandiamide (DCDA) – a simple molecular precursor – in a eutectic salt melt of lithium chloride and potassium chloride. The extent of condensation, namely next to complete conversion of all reactive end groups, was verified by elemental microanalysis and vibrational spectroscopy. TEM- and SEM-measurements gave detailed insight into the well-defined morphology of these organic crystals, which are not based on 0D or 1D constituents like known molecular or short-chain polymeric crystals but on the packing motif of extended 2D frameworks. The proposed crystal structure of this g-C3N4 species was derived in analogy to graphite by means of extensive powder XRD studies, indexing and refinement. It is based on sheets of hexagonally arranged s-heptazine (C6N7) units that are held together by covalent bonds between C and N atoms. These sheets stack in a graphitic, staggered fashion adopting an AB-motif, as corroborated by powder X-ray diffractometry and high-resolution transmission electron microscopy. This study was contrasted with one of many popular – yet unsuccessful – approaches in the last 30 years of scientific literature to perform the condensation of an extended carbon nitride species through synthesis in the bulk. The second section expands the repertoire of available salt melts introducing the lithium bromide and potassium bromide eutectic as an excellent medium to obtain a new phase of graphitic carbon nitride. The combination of SEM, TEM, PXRD and electron diffraction reveals that the new graphitic carbon nitride phase stacks in an ABA’ motif forming unprecedentedly large crystals. This section seizes the notion of the preceding chapter, that condensation in a eutectic salt melt is the key to obtain a high degree of conversion mainly through a solvatory effect. At the close of this chapter ionothermal synthesis is seen established as a powerful tool to overcome the inherent kinetic problems of solid state reactions such as incomplete polymerisation and condensation in the bulk especially when the temperature requirement of the reaction in question falls into the proverbial “no man’s land” of classical solvents, i.e. above 250 to 300 °C. The following section puts the claim to the test, that the crystalline carbon nitrides obtained from a salt melt are indeed graphitic. A typical property of graphite – namely the accessibility of its interplanar space for guest molecules – is transferred to the graphitic carbon nitride system. Metallic potassium and graphitic carbon nitride are converted to give the potassium intercalation compound, K(C6N8)3 designated according to its stoichiometry and proposed crystal structure. Reaction of the intercalate with aqueous solvents triggers the exfoliation of the graphitic carbon nitride material and – for the first time – enables the access of singular (or multiple) carbon nitride sheets analogous to graphene as seen in the formation of sheets, bundles and scrolls of carbon nitride in TEM imaging. The thus exfoliated sheets form a stable, strongly fluorescent solution in aqueous media, which shows no sign in UV/Vis spectroscopy that the aromaticity of individual sheets was subject to degradation. The final section expands on the mechanism underlying the formation of graphitic carbon nitride by literally expanding the distance between the covalently linked heptazine units which constitute these materials. A close examination of all proposed reaction mechanisms to-date in the light of exhaustive DSC/MS experiments highlights the possibility that the heptazine unit can be formed from smaller molecules, even if some of the designated leaving groups (such as ammonia) are substituted by an element, R, which later on remains linked to the nascent heptazine. Furthermore, it is suggested that the key functional groups in the process are the triazine- (Tz) and the carbonitrile- (CN) group. On the basis of these assumptions, molecular precursors are tailored which encompass all necessary functional groups to form a central heptazine unit of threefold, planar symmetry and then still retain outward functionalities for self-propagated condensation in all three directions. Two model systems based on a para-aryl (ArCNTz) and para-biphenyl (BiPhCNTz) precursors are devised via a facile synthetic procedure and then condensed in an ionothermal process to yield the heptazine based frameworks, HBF-1 and HBF-2. Due to the structural motifs of their molecular precursors, individual sheets of HBF-1 and HBF-2 span cavities of 14.2 Å and 23.0 Å respectively which makes both materials attractive as potential organic zeolites. Crystallographic analysis confirms the formation of ABA’ layered, graphitic systems, and the extent of condensation is confirmed as next-to-perfect by elemental analysis and vibrational spectroscopy.
Recent years witnessed a vast advent of stalagmites as palaeoclimate archives. The multitude of geochemical and physical proxies and a promise of a precise and accurate age model greatly appeal to palaeoclimatologists. Although substantial progress was made in speleothem-based palaeoclimate research and despite high-resolution records from low-latitudinal regions, proving that palaeo-environmental changes can be archived on sub-annual to millennial time scales our comprehension of climate dynamics is still fragmentary. This is in particular true for the summer monsoon system on the Indian subcontinent. The Indian summer monsoon (ISM) is an integral part of the intertropical convergence zone (ITCZ). As this rainfall belt migrates northward during boreal summer, it brings monsoonal rainfall. ISM strength depends however on a variety of factors, including snow cover in Central Asia and oceanic conditions in the Indic and Pacific. Presently, many of the factors influencing the ISM are known, though their exact forcing mechanism and mutual relations remain ambiguous. Attempts to make an accurate prediction of rainfall intensity and frequency and drought recurrence, which is extremely important for South Asian countries, resemble a puzzle game; all interaction need to fall into the right place to obtain a complete picture. My thesis aims to create a faithful picture of climate change in India, covering the last 11,000 ka. NE India represents a key region for the Bay of Bengal (BoB) branch of the ISM, as it is here where the monsoon splits into a northwestward and a northeastward directed arm. The Meghalaya Plateau is the first barrier for northward moving air masses and receives excessive summer rainfall, while the winter season is very dry. The proximity of Meghalaya to the Tibetan Plateau on the one hand and the BoB on the other hand make the study area a key location for investigating the interaction between different forcings that governs the ISM. A basis for the interpretation of palaeoclimate records, and a first important outcome of my thesis is a conceptual model which explains the observed pattern of seasonal changes in stable isotopes (d18O and d2H) in rainfall. I show that although in tropical and subtropical regions the amount effect is commonly called to explain strongly depleted isotope values during enhanced rainfall, alone it cannot account for observed rainwater isotope variability in Meghalaya. Monitoring of rainwater isotopes shows no expected negative correlation between precipitation amount and d18O of rainfall. In turn I find evidence that the runoff from high elevations carries an inherited isotopic signature into the BoB, where during the ISM season the freshwater builds a strongly depleted plume on top of the marine water. The vapor originating from this plume is likely to memorize' and transmit further very negative d18O values. The lack of data does not allow for quantication of this plume effect' on isotopes in rainfall over Meghalaya but I suggest that it varies on seasonal to millennial timescales, depending on the runoff amount and source characteristics. The focal point of my thesis is the extraction of climatic signals archived in stalagmites from NE India. High uranium concentration in the stalagmites ensured excellent age control required for successful high-resolution climate reconstructions. Stable isotope (d18O and d13C) and grey-scale data allow unprecedented insights into millennial to seasonal dynamics of the summer and winter monsoon in NE India. ISM strength (i. e. rainfall amount) is recorded in changes in d18Ostalagmites. The d13C signal, reflecting drip rate changes, renders a powerful proxy for dry season conditions, and shows similarities to temperature-related changes on the Tibetan Plateau. A sub-annual grey-scale profile supports a concept of lower drip rate and slower stalagmite growth during dry conditions. During the Holocene, ISM followed a millennial-scale decrease of insolation, with decadal to centennial failures resulting from atmospheric changes. The period of maximum rainfall and enhanced seasonality corresponds to the Holocene Thermal Optimum observed in Europe. After a phase of rather stable conditions, 4.5 kyr ago, the strengthening ENSO system dominated the ISM. Strong El Nino events weakened the ISM, especially when in concert with positive Indian Ocean dipole events. The strongest droughts of the last 11 kyr are recorded during the past 2 kyr. Using the advantage of a well-dated stalagmite record at hand I tested the application of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) to detect sub-annual to sub-decadal changes in element concentrations in stalagmites. The development of a large ablation cell allows for ablating sample slabs of up to 22 cm total length. Each analyzed element is a potential proxy for different climatic parameters. Combining my previous results with the LAICP- MS-generated data shows that element concentration depends not only on rainfall amount and associated leaching from the soil. Additional factors, like biological activity and hydrogeochemical conditions in the soil and vadose zone can eventually affect the element content in drip water and in stalagmites. I present a theoretical conceptual model for my study site to explain how climatic signals can be transmitted and archived in stalagmite carbonate. Further, I establish a first 1500 year long element record, reconstructing rainfall variability. Additionally, I hypothesize that volcanic eruptions, producing large amounts of sulfuric acid, can influence soil acidity and hence element mobilization.
Submarine landslides can generate local tsunamis posing a hazard to human lives and coastal facilities. Two major related problems are: (i) quantitative estimation of tsunami hazard and (ii) early detection of the most dangerous landslides. This thesis focuses on both those issues by providing numerical modeling of landslide-induced tsunamis and by suggesting and justifying a new method for fast detection of tsunamigenic landslides by means of tiltmeters. Due to the proximity to the Sunda subduction zone, Indonesian coasts are prone to earthquake, but also landslide tsunamis. The aim of the GITEWS-project (German-Indonesian Tsunami Early Warning System) is to provide fast and reliable tsunami warnings, but also to deepen the knowledge about tsunami hazards. New bathymetric data at the Sunda Arc provide the opportunity to evaluate the hazard potential of landslide tsunamis for the adjacent Indonesian islands. I present nine large mass movements in proximity to Sumatra, Java, Sumbawa and Sumba, whereof the largest event displaced 20 km³ of sediments. Using numerical modeling, I compute the generated tsunami of each event, its propagation and runup at the coast. Moreover, I investigate the age of the largest slope failures by relating them to the Great 1977 Sumba earthquake. Continental slopes off northwest Europe are well known for their history of huge underwater landslides. The current geological situation west of Spitsbergen is comparable to the continental margin off Norway after the last glaciation, when the large tsunamigenic Storegga slide took place. The influence of Arctic warming on the stability of the Svalbard glacial margin is discussed. Based on new geophysical data, I present four possible landslide scenarios and compute the generated tsunamis. Waves of 6 m height would be capable of reaching northwest Europe threatening coastal areas. I present a novel technique to detect large submarine landslides using an array of tiltmeters, as a possible tool in future tsunami early warning systems. The dislocation of a large amount of sediment during a landslide produces a permanent elastic response of the earth. I analyze this response with a mathematical model and calculate the theoretical tilt signal. Applications to the hypothetical Spitsbergen event and the historical Storegga slide show tilt signals exceeding 1000 nrad. The amplitude of landslide tsunamis is controlled by the product of slide volume and maximal velocity (slide tsunamigenic potential). I introduce an inversion routine that provides slide location and tsunamigenic potential, based on tiltmeter measurements. The accuracy of the inversion and of the estimated tsunami height near the coast depends on the noise level of tiltmeter measurements, the distance of tiltmeters from the slide, and the slide tsunamigenic potential. Finally, I estimate the applicability scope of this method by employing it to known landslide events worldwide.
Normality is one of the defining categories of our society. Statistics of all kinds play a crucial part in establishing the normal. Computers, on the other hand, have a very close connection to statistics as the digital world is a statistical one in itself. In a multitude of games statistics are used as an element of gameplay. In this perspective, games can be regarded as a training in self-normalization. However, it is still questionable whether this leads to a genuine production of normality.
Controlling interactions in synthetic polymers as precisely as in proteins would have a strong impact on polymer science. Advanced structural and functional control can lead to rational design of, integrated nano- and microstructures. To achieve this, properties of monomer sequence defined oligopeptides were exploited. Through their incorporation as monodisperse segments into synthetic polymers we learned in recent four years how to program the structure formation of polymers, to adjust and exploit interactions in such polymers, to control inorganic-organic interfaces in fiber composites and induce structure in Biomacromolecules like DNA for biomedical applications.
For three small, mountainous catchments in Germany two medium-range forecast systems are compared that predict precipitation for up to 5 days in advance. One system is composed of the global German weather service (DWD) model, GME, which is dynamically downscaled using the COSMO-EU regional model. The other system is an empirical (expanded) downscaling of the ECMWF model IFS. Forecasts are verified against multi-year daily observations, by applying standard skill scores to events of specified intensity. All event classes are skillfully predicted by the empirical system for up to five days lead time. For the available prediction range of one to two days it is superior to the dynamical system.