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Nanostructured inorganic materials are routinely synthesized by the use of templates. Depending on the synthesis conditions of the product material, either “soft” or “hard” templates can be applied. For sol-gel processes, usually “soft” templating techniques are employed, while “hard” templates are used for high temperature synthesis pathways. In classical templating approaches, the template has the unique role of structure directing agent, in the sense that it is not participating to the chemical formation of the resulting material. This work investigates a new templating pathway to nanostructured materials, where the template is also a reagent in the formation of the final material. This concept is described as “reactive templating” and opens a synthetic path toward materials which cannot be synthesised on a nanometre scale by classical templating approaches. Metal nitrides are such kind of materials. They are usually produced by the conversion of metals or metal oxides in ammonia flow at high temperature (T > 1000°C), which make the application of classical templating techniques difficult. Graphitic carbon nitride, g-C3N4, despite its fundamental and theoretical importance, is probably one of the most promising materials to complement carbon in material science and many efforts are put in the synthesis of this material. A simple polyaddition/elimination reaction path at high temperature (T = 550°C) allows the polymerisation of cyanamide toward graphitic carbon nitride solids. By hard templating, using nanostructured silica or aluminium oxide as nanotemplates, a variety of nanostructured graphitic carbon nitrides such as nanorods, nanotubes, meso- and macroporous powders could be obtained by nanocasting or nanocoating. Due to the special semi-conducting properties of the graphitic carbon nitride matrix, the nanostructured graphitic carbon nitrides show unexpected catalytic activity for the activation of benzene in Friedel-Crafts type reactions, making this material an interesting metal free catalyst. Furthermore, due to the chemical composition of g-C3N4 and the fact that it is totally decomposed at temperatures between 600°C and 800°C even under inert atmosphere, g-C3N4 was shown to be a good nitrogen donor for the synthesis of early transition metal nitrides at high temperatures. Thus using the nanostructured carbon nitrides as “reactive templates” or “nanoreactors”, various metal nitride nanostructures, such as nanoparticles and porous frameworks could be obtained at high temperature. In this approach the carbon nitride nanostructure played both the role of the nitrogen source and of the exotemplate, imprinting its size and shape to the resulting metal nitride nanostructure.
The Earth’s shallow subsurface with sedimentary cover acts as a waveguide to any incoming wavefield. Within the framework of my thesis, I focused on the characterization of this shallow subsurface within tens to few hundreds of meters of sediment cover. I imaged the seismic 1D shear wave velocity (and possibly the 1D compressional wave velocity). This information is not only required for any seismic risk assessment, geotechnical engineering or microzonation activities, but also for exploration and global seismology where site effects are often neglected in seismic waveform modeling.
First, the conventional frequency-wavenumber (f - k) technique is used to derive the dispersion characteristic of the propagating surface waves recorded using distinct arrays of seismometers in 1D and 2D configurations. Further, the cross-correlation technique is applied to seismic array data to estimate the Green’s function between receivers pairs combination assuming one is the source and the other the receiver. With the consideration of a 1D media, the estimated cross-correlation Green’s functions are sorted with interstation distance in a virtual 1D active seismic experiment. The f - k technique is then used to estimate the dispersion curves. This integrated analysis is important for the interpretation of a large bandwidth of the phase velocity dispersion curves and therefore improving the resolution of the estimated 1D Vs profile.
Second, the new theoretical approach based on the Diffuse Field Assumption (DFA) is used for the interpretation of the observed microtremors H/V spectral ratio. The theory is further extended in this research work to include not only the interpretation of the H/V measured at the surface, but also the H/V measured at depths and in marine environments. A modeling and inversion of synthetic H/V spectral ratio curves on simple predefined geological structures shows an almost perfect recovery of the model parameters (mainly Vs and to a lesser extent Vp). These results are obtained after information from a receiver at depth has been considered in the inversion.
Finally, the Rayleigh wave phase velocity information, estimated from array data, and the H/V(z, f) spectral ratio, estimated from a single station data, are combined and inverted for the velocity profile information. Obtained results indicate an improved depth resolution in comparison to estimations using the phase velocity dispersion curves only. The overall estimated sediment thickness is comparable to estimations obtained by inverting the full micortremor H/V spectral ratio.
The study of outcrop modeling is located at the interface between two fields of expertise, Sedimentology and Computing Geoscience, which respectively investigates and simulates geological heterogeneity observed in the sedimentary record. During the last past years, modeling tools and techniques were constantly improved. In parallel, the study of Phanerozoic carbonate deposits emphasized the common occurrence of a random facies distribution along single depositional domain. Although both fields of expertise are intrinsically linked during outcrop simulation, their respective advances have not been combined in literature to enhance carbonate modeling studies. The present study re-examines the modeling strategy adapted to the simulation of shallow-water carbonate systems, based on a close relationship between field sedimentology and modeling capabilities. In the present study, the evaluation of three commonly used algorithms Truncated Gaussian Simulation (TGSim), Sequential Indicator Simulation (SISim), and Indicator Kriging (IK), were performed for the first time using visual and quantitative comparisons on an ideally suited carbonate outcrop. The results show that the heterogeneity of carbonate rocks cannot be fully simulated using one single algorithm. The operating mode of each algorithm involves capabilities as well as drawbacks that are not capable to match all field observations carried out across the modeling area. Two end members in the spectrum of carbonate depositional settings, a low-angle Jurassic ramp (High Atlas, Morocco) and a Triassic isolated platform (Dolomites, Italy), were investigated to obtain a complete overview of the geological heterogeneity in shallow-water carbonate systems. Field sedimentology and statistical analysis performed on the type, morphology, distribution, and association of carbonate bodies and combined with palaeodepositional reconstructions, emphasize similar results. At the basin scale (x 1 km), facies association, composed of facies recording similar depositional conditions, displays linear and ordered transitions between depositional domains. Contrarily, at the bedding scale (x 0.1 km), individual lithofacies type shows a mosaic-like distribution consisting of an arrangement of spatially independent lithofacies bodies along the depositional profile. The increase of spatial disorder from the basin to bedding scale results from the influence of autocyclic factors on the transport and deposition of carbonate sediments. Scale-dependent types of carbonate heterogeneity are linked with the evaluation of algorithms in order to establish a modeling strategy that considers both the sedimentary characteristics of the outcrop and the modeling capabilities. A surface-based modeling approach was used to model depositional sequences. Facies associations were populated using TGSim to preserve ordered trends between depositional domains. At the lithofacies scale, a fully stochastic approach with SISim was applied to simulate a mosaic-like lithofacies distribution. This new workflow is designed to improve the simulation of carbonate rocks, based on the modeling of each scale of heterogeneity individually. Contrarily to simulation methods applied in literature, the present study considers that the use of one single simulation technique is unlikely to correctly model the natural patterns and variability of carbonate rocks. The implementation of different techniques customized for each level of the stratigraphic hierarchy provides the essential computing flexibility to model carbonate systems. Closer feedback between advances carried out in the field of Sedimentology and Computing Geoscience should be promoted during future outcrop simulations for the enhancement of 3-D geological models.
Today, near-surface investigations are frequently conducted using non-destructive or minimally invasive methods of applied geophysics, particularly in the fields of civil engineering, archaeology, geology, and hydrology. One field that plays an increasingly central role in research and engineering is the examination of sedimentary environments, for example, for characterizing near-surface groundwater systems. A commonly employed method in this context is ground-penetrating radar (GPR). In this technique, short electromagnetic pulses are emitted into the subsurface by an antenna, which are then reflected, refracted, or scattered at contrasts in electromagnetic properties (such as the water table). A receiving antenna records these signals in terms of their amplitudes and travel times. Analysis of the recorded signals allows for inferences about the subsurface, such as the depth of the groundwater table or the composition and characteristics of near-surface sediment layers. Due to the high resolution of the GPR method and continuous technological advancements, GPR data acquisition is increasingly performed in three-dimensional (3D) fashion today.
Despite the considerable temporal and technical efforts involved in data acquisition and processing, the resulting 3D data sets (providing high-resolution images of the subsurface) are typically interpreted manually. This is generally an extremely time-consuming analysis step. Therefore, representative 2D sections highlighting distinctive reflection structures are often selected from the 3D data set. Regions showing similar structures are then grouped into so-called radar facies. The results obtained from 2D sections are considered representative of the entire investigated area. Interpretations conducted in this manner are often incomplete and highly dependent on the expertise of the interpreters, making them generally non-reproducible.
A promising alternative or complement to manual interpretation is the use of GPR attributes. Instead of using the recorded data directly, derived quantities characterizing distinctive reflection structures in 3D are applied for interpretation. Using various field and synthetic data sets, this thesis investigates which attributes are particularly suitable for this purpose. Additionally, the study demonstrates how selected attributes can be utilized through specific processing and classification methods to create 3D facies models. The ability to generate attribute-based 3D GPR facies models allows for partially automated and more efficient interpretations in the future. Furthermore, the results obtained in this manner describe the subsurface in a reproducible and more comprehensive manner than what has typically been achievable through manual interpretation methods.
3D from 2D touch
(2013)
While interaction with computers used to be dominated by mice and keyboards, new types of sensors now allow users to interact through touch, speech, or using their whole body in 3D space. These new interaction modalities are often referred to as "natural user interfaces" or "NUIs." While 2D NUIs have experienced major success on billions of mobile touch devices sold, 3D NUI systems have so far been unable to deliver a mobile form factor, mainly due to their use of cameras. The fact that cameras require a certain distance from the capture volume has prevented 3D NUI systems from reaching the flat form factor mobile users expect. In this dissertation, we address this issue by sensing 3D input using flat 2D sensors. The systems we present observe the input from 3D objects as 2D imprints upon physical contact. By sampling these imprints at very high resolutions, we obtain the objects' textures. In some cases, a texture uniquely identifies a biometric feature, such as the user's fingerprint. In other cases, an imprint stems from the user's clothing, such as when walking on multitouch floors. By analyzing from which part of the 3D object the 2D imprint results, we reconstruct the object's pose in 3D space. While our main contribution is a general approach to sensing 3D input on 2D sensors upon physical contact, we also demonstrate three applications of our approach. (1) We present high-accuracy touch devices that allow users to reliably touch targets that are a third of the size of those on current touch devices. We show that different users and 3D finger poses systematically affect touch sensing, which current devices perceive as random input noise. We introduce a model for touch that compensates for this systematic effect by deriving the 3D finger pose and the user's identity from each touch imprint. We then investigate this systematic effect in detail and explore how users conceptually touch targets. Our findings indicate that users aim by aligning visual features of their fingers with the target. We present a visual model for touch input that eliminates virtually all systematic effects on touch accuracy. (2) From each touch, we identify users biometrically by analyzing their fingerprints. Our prototype Fiberio integrates fingerprint scanning and a display into the same flat surface, solving a long-standing problem in human-computer interaction: secure authentication on touchscreens. Sensing 3D input and authenticating users upon touch allows Fiberio to implement a variety of applications that traditionally require the bulky setups of current 3D NUI systems. (3) To demonstrate the versatility of 3D reconstruction on larger touch surfaces, we present a high-resolution pressure-sensitive floor that resolves the texture of objects upon touch. Using the same principles as before, our system GravitySpace analyzes all imprints and identifies users based on their shoe soles, detects furniture, and enables accurate touch input using feet. By classifying all imprints, GravitySpace detects the users' body parts that are in contact with the floor and then reconstructs their 3D body poses using inverse kinematics. GravitySpace thus enables a range of applications for future 3D NUI systems based on a flat sensor, such as smart rooms in future homes. We conclude this dissertation by projecting into the future of mobile devices. Focusing on the mobility aspect of our work, we explore how NUI devices may one day augment users directly in the form of implanted devices.
Hepcidin-25 (Hep-25) plays a crucial role in the control of iron homeostasis. Since the dysfunction of the hepcidin pathway leads to multiple diseases as a result of iron imbalance, hepcidin represents a potential target for the diagnosis and treatment of disorders of iron metabolism. Despite intense research in the last decade targeted at developing a selective immunoassay for iron disorder diagnosis and treatment and better understanding the ferroportin-hepcidin interaction, questions remain. The key to resolving these underlying questions is acquiring exact knowledge of the 3D structure of native Hep-25. Since it was determined that the N-terminus, which is responsible for the bioactivity of Hep-25, contains a small Cu(II)-binding site known as the ATCUN motif, it was assumed that the Hep-25-Cu(II) complex is the native, bioactive form of the hepcidin. This structure has thus far not been elucidated in detail. Owing to the lack of structural information on metal-bound Hep-25, little is known about its possible biological role in iron metabolism. Therefore, this work is focused on structurally characterizing the metal-bound Hep-25 by NMR spectroscopy and molecular dynamics simulations. For the present work, a protocol was developed to prepare and purify properly folded Hep-25 in high quantities. In order to overcome the low solubility of Hep-25 at neutral pH, we introduced the C-terminal DEDEDE solubility tag. The metal binding was investigated through a series of NMR spectroscopic experiments to identify the most affected amino acids that mediate metal coordination. Based on the obtained NMR data, a structural calculation was performed in order to generate a model structure of the Hep-25-Ni(II) complex. The DEDEDE tag was excluded from the structural calculation due to a lack of NMR restraints. The dynamic nature and fast exchange of some of the amide protons with solvent reduced the overall number of NMR restraints needed for a high-quality structure. The NMR data revealed that the 20 Cterminal Hep-25 amino acids experienced no significant conformational changes, compared to published results, as a result of a pH change from pH 3 to pH 7 and metal binding. A 3D model of the Hep-25-Ni(II) complex was constructed from NMR data recorded for the hexapeptideNi(II) complex and Hep-25-DEDEDE-Ni(II) complex in combination with the fixed conformation of 19 C-terminal amino acids. The NMR data of the Hep-25-DEDEDE-Ni(II) complex indicates that the ATCUN motif moves independently from the rest of the structure. The 3D model structure of the metal-bound Hep-25 allows for future works to elucidate hepcidin’s interaction with its receptor ferroportin and should serve as a starting point for the development of antibodies with improved selectivity.
The scientific drilling campaign PALEOVAN was conducted in the summer of 2010 and was part of the international continental drilling programme (ICDP). The main goal of the campaign was the recovery of a sensitive climate archive in the East of Anatolia. Lacustrine deposits underneath the lake floor of ‘Lake Van’ constitute this archive. The drilled core material was recovered from two locations: the Ahlat Ridge and the Northern Basin. A composite core was constructed from cored material of seven parallel boreholes at the Ahlat Ridge and covers an almost complete lacustrine history of Lake Van. The composite record offered sensitive climate proxies such as variations of total organic carbon, K/Ca ratios, or a relative abundance of arboreal pollen. These proxies revealed patterns that are similar to climate proxy variations from Greenland ice cores. Climate variations in Greenland ice cores have been dated by modelling the timing of orbital forces to affect the climate. Volatiles from melted ice aliquots are often taken as high-resolution proxies and provide a base for fitting the according temporal models.
The ICDP PALEOVAN scientific team fitted proxy data from the lacustrine drilling record to ice core data and constructed an age model. Embedded volcaniclastic layers had to be dated radiometrically in order to provide independent age constraints to the climate-stratigraphic age model. Solving this task by an application of the 40Ar/39Ar method was the main objective of this thesis. Earlier efforts to apply the 40Ar/39Ar dating resulted in inaccuracies that could not be explained satisfactorily.
The absence of K-rich feldspars in suitable tephra layers implied that feldspar crystals needed to be 500 μm in size minimum, in order to apply single-crystal 40Ar/39Ar dating. Some of the samples did not contain any of these grain sizes or only very few crystals of that size. In order to overcome this problem this study applied a combined single-crystal and multi-crystal approach with different crystal fractions from the same sample. The preferred method of a stepwise heating analysis of an aliquot of feldspar crystals has been applied to three samples. The Na-rich crystals and their young geological age required 20 mg of inclusion-free, non-corroded feldspars. Small sample volumes (usually 25 % aliquots of 5 cm3 of sample material – a spoon full of tephra) and the widespread presence of melt-inclusion led to the application of combined single- and multigrain total fusion analyses. 40Ar/39Ar analyses on single crystals have the advantage of being able to monitor the presence of excess 40Ar and detrital or xenocrystic contamination in the samples. Multigrain analyses may hide the effects from these obstacles. The results from the multigrain analyses are therefore discussed with respect to the findings from the respective cogenetic single crystal ages. Some of the samples in this study were dated by 40Ar/39Ar on feldspars on multigrain separates and (if available) in combination with only a few single crystals. 40Ar/39Ar ages from two of the samples deviated statistically from the age model. All other samples resulted in identical ages. The deviations displayed older ages than those obtained from the age model. t-Tests compared radiometric ages with available age control points from various proxies and from the relative paleointensity of the earth magnetic field within a stratigraphic range of ± 10 m. Concordant age control points from different relative chronometers indicated that deviations are a result of erroneous 40Ar/39Ar ages. The thesis argues two potential reasons for these ages: (1) the irregular appearance of 40Ar from rare melt- and fluid- inclusions and (2) the contamination of the samples with older crystals due to a rapid combination of assimilation and ejection.
Another aliquot of feldspar crystals that underwent separation for the application of 40Ar/39Ar dating was investigated for geochemical inhomogeneities. Magmatic zoning is ubiquitous in the volcaniclastic feldspar crystals. Four different types of magmatic zoning were detected. The zoning types are compositional zoning (C-type zoning), pseudo-oscillatory zoning of trace ele- ment concentrations (PO-type zoning), chaotic and patchy zoning of major and trace element concentrations (R-type zoning) and concentric zoning of trace elements (CC-type zoning). Sam- ples that deviated in 40Ar/39Ar ages showed C-type zoning, R-type zoning or a mix of different types of zoning (C-type and PO-type). Feldspars showing PO-type zoning typically represent the smallest grain size fractions in the samples. The constant major element compositions of these crystals are interpreted to represent the latest stages in the compositional evolution of feldspars in a peralkaline melt. PO-type crystals contain less melt- inclusions than other zoning types and are rarely corroded. This thesis concludes that feldspars that show PO-type zoning are most promising chronometers for the 40Ar/39Ar method, if samples provide mixed zoning types of Quaternary anorthoclase feldspars.
Five samples were dated by applying the 40Ar/39Ar method to volcanic glass. High fractions of atmospheric Ar (typically > 98%) significantly hampered the precision of the 40Ar/39Ar ages and resulted in rough age estimates that widely overlap the age model. Ar isotopes indicated that the glasses bore a chorine-rich Ar-end member. The chlorine-derived 38Ar indicated chlorine-rich fluid-inclusions or the hydration of the volcanic glass shards. This indication strengthened the evidence that irregularly distributed melt-inclusions and thus irregular distributed excess 40Ar influenced the problematic feldspar 40Ar/39Ar ages. Whether a connection between a corrected initial 40Ar/36Ar ratio from glasses to the 40Ar/36Ar ratios from pore waters exists remains unclear.
This thesis offers another age model, which is similarly based on the interpolation of the temporal tie points from geophysical and climate-stratigraphic data. The model used a PCHIP- interpolation (piecewise cubic hermite interpolating polynomial) whereas the older age model used a spline-interpolation. Samples that match in ages from 40Ar/39Ar dating of feldspars with the earlier published age model were additionally assigned with an age from the PCHIP- interpolation. These modelled ages allowed a recalculation of the Alder Creek sanidine mineral standard. The climate-stratigraphic calibration of an 40Ar/39Ar mineral standard proved that the age versus depth interpolations from PAELOVAN drilling cores were accurate, and that the applied chronometers recorded the temporal evolution of Lake Van synchronously.
Petrochemical discrimination of the sampled volcaniclastic material is also given in this thesis. 41 from 57 sampled volcaniclastic layers indicate Nemrut as their provenance. Criteria that served for the provenance assignment are provided and reviewed critically. Detailed correlations of selected PALEOVAN volcaniclastics to onshore samples that were described in detail by earlier studies are also discussed. The sampled volcaniclastics dominantly have a thickness of < 40 cm and have been ejected by small to medium sized eruptions. Onshore deposits from these types of eruptions are potentially eroded due to predominant strong winds on Nemrut and Süphan slopes. An exact correlation with the data presented here is therefore equivocal or not possible at all.
Deviating feldspar 40Ar/39Ar ages can possibly be explained by inherited 40Ar from feldspar xenocrysts contaminating the samples. In order to test this hypothesis diffusion couples of Ba were investigated in compositionally zoned feldspar crystals. The diffusive behaviour of Ba in feldspar is known, and gradients in the changing concentrations allowed for the calculation of the duration of the crystal’s magmatic development since the formation of the zoning interface. Durations were compared with degassing scenarios that model the Ar-loss during assimilation and subsequent ejection of the xenocrystals. Diffusive equilibration of the contrasting Ba concentrations is assumed to generate maximum durations as the gradient could have been developed in several growth and heating stages. The modelling does not show any indication of an involvement of inherited 40Ar in any of the deviating samples. However, the analytical set-up represents the lower limit of the required spatial resolution. Therefore, it cannot be excluded that the degassing modelling relies on a significant overestimation of the maximum duration of the magmatic history. Nevertheless, the modelling of xenocrystal degassing evidences that the irregular incorporation of excess 40Ar by melt- and fluid inclusions represents the most critical problem that needs to be overcome in dating volcaniclastic feldspars from the PALEOVAN drill cores. This thesis provides the complete background in generating and presenting 40Ar/39Ar ages that are compared to age data from a climate-stratigraphic model. Deviations are identified statistically and then discussed in order to find explanations from the age model and/or from 40Ar/39Ar geochronology. Most of the PALEOVAN stratigraphy provides several chronometers that have been proven for their synchronicity. Lacustrine deposits from Lake Van represent a key archive for reconstructing climate evolution in the eastern Mediterranean and in the Near East. The PALEOVAN record offers a climate-stratigraphic age model with a remarkable accuracy and resolution.
The potential increase in frequency and magnitude of extreme floods is currently discussed in terms of global warming and the intensification of the hydrological cycle. The profound knowledge of past natural variability of floods is of utmost importance in order to assess flood risk for the future. Since instrumental flood series cover only the last ~150 years, other approaches to reconstruct historical and pre-historical flood events are needed. Annually laminated (varved) lake sediments are meaningful natural geoarchives because they provide continuous records of environmental changes > 10000 years down to a seasonal resolution. Since lake basins additionally act as natural sediment traps, the riverine sediment supply, which is preserved as detrital event layers in the lake sediments, can be used as a proxy for extreme discharge events. Within my thesis I examined a ~ 8.50 m long sedimentary record from the pre-Alpine Lake Mondsee (Northeast European Alps), which covered the last 7000 years. This sediment record consists of calcite varves and intercalated detrital layers, which range in thickness from 0.05 to 32 mm. Detrital layer deposition was analysed by a combined method of microfacies analysis via thin sections, Scanning Electron Microscopy (SEM), μX-ray fluorescence (μXRF) scanning and magnetic susceptibility. This approach allows characterizing individual detrital event layers and assigning a corresponding input mechanism and catchment. Based on varve counting and controlled by 14C age dates, the main goals of this thesis are (i) to identify seasonal runoff processes, which lead to significant sediment supply from the catchment into the lake basin and (ii) to investigate flood frequency under changing climate boundary conditions. This thesis follows a line of different time slices, presenting an integrative approach linking instrumental and historical flood data from Lake Mondsee in order to evaluate the flood record inferred from Lake Mondsee sediments. The investigation of eleven short cores covering the last 100 years reveals the abundance of 12 detrital layers. Therein, two types of detrital layers are distinguished by grain size, geochemical composition and distribution pattern within the lake basin. Detrital layers, which are enriched in siliciclastic and dolomitic material, reveal sediment supply from the Flysch sediments and Northern Calcareous Alps into the lake basin. These layers are thicker in the northern lake basin (0.1-3.9 mm) and thinner in the southern lake basin (0.05-1.6 mm). Detrital layers, which are enriched in dolomitic components forming graded detrital layers (turbidites), indicate the provenance from the Northern Calcareous Alps. These layers are generally thicker (0.65-32 mm) and are solely recorded within the southern lake basin. In comparison with instrumental data, thicker graded layers result from local debris flow events in summer, whereas thin layers are deposited during regional flood events in spring/summer. Extreme summer floods as reported from flood layer deposition are principally caused by cyclonic activity from the Mediterranean Sea, e.g. July 1954, July 1997 and August 2002. During the last two millennia, Lake Mondsee sediments reveal two significant flood intervals with decadal-scale flood episodes, during the Dark Ages Cold Period (DACP) and the transition from the Medieval Climate Anomaly (MCA) into the Little Ice Age (LIA) suggesting a linkage of transition to climate cooling and summer flood recurrences in the Northeastern Alps. In contrast, intermediate or decreased flood episodes appeared during the MWP and the LIA. This indicates a non-straightforward relationship between temperature and flood recurrence, suggesting higher cyclonic activity during climate transition in the Northeast Alps. The 7000-year flood chronology reveals 47 debris flows and 269 floods, with increased flood activity shifting around 3500 and 1500 varve yr BP (varve yr BP = varve years before present, before present = AD 1950). This significant increase in flood activity shows a coincidence with millennial-scale climate cooling that is reported from main Alpine glacier advances and lower tree lines in the European Alps since about 3300 cal. yr BP (calibrated years before present). Despite relatively low flood occurrence prior to 1500 varve yr BP, floods at Lake Mondsee could have also influenced human life in early Neolithic lake dwellings (5750-4750 cal. yr BP). While the first lake dwellings were constructed on wetlands, the later lake dwellings were built on piles in the water suggesting an early flood risk adaptation of humans and/or a general change of the Late Neolithic Culture of lake-dwellers because of socio-economic reasons. However, a direct relationship between the final abandonment of the lake dwellings and higher flood frequencies is not evidenced.
Data stream processing systems (DSPSs) are a key enabler to integrate continuously generated data, such as sensor measurements, into enterprise applications. DSPSs allow to steadily analyze information from data streams, e.g., to monitor manufacturing processes and enable fast reactions to anomalous behavior. Moreover, DSPSs continuously filter, sample, and aggregate incoming streams of data, which reduces the data size, and thus data storage costs.
The growing volumes of generated data have increased the demand for high-performance DSPSs, leading to a higher interest in these systems and to the development of new DSPSs. While having more DSPSs is favorable for users as it allows choosing the system that satisfies their requirements the most, it also introduces the challenge of identifying the most suitable DSPS regarding current needs as well as future demands. Having a solution to this challenge is important because replacements of DSPSs require the costly re-writing of applications if no abstraction layer is used for application development. However, quantifying performance differences between DSPSs is a difficult task. Existing benchmarks fail to integrate all core functionalities of DSPSs and lack tool support, which hinders objective result comparisons. Moreover, no current benchmark covers the combination of streaming data with existing structured business data, which is particularly relevant for companies.
This thesis proposes a performance benchmark for enterprise stream processing called ESPBench. With enterprise stream processing, we refer to the combination of streaming and structured business data. Our benchmark design represents real-world scenarios and allows for an objective result comparison as well as scaling of data. The defined benchmark query set covers all core functionalities of DSPSs. The benchmark toolkit automates the entire benchmark process and provides important features, such as query result validation and a configurable data ingestion rate.
To validate ESPBench and to ease the use of the benchmark, we propose an example implementation of the ESPBench queries leveraging the Apache Beam software development kit (SDK). The Apache Beam SDK is an abstraction layer designed for developing stream processing applications that is applied in academia as well as enterprise contexts. It allows to run the defined applications on any of the supported DSPSs. The performance impact of Apache Beam is studied in this dissertation as well. The results show that there is a significant influence that differs among DSPSs and stream processing applications. For validating ESPBench, we use the example implementation of the ESPBench queries developed using the Apache Beam SDK. We benchmark the implemented queries executed on three modern DSPSs: Apache Flink, Apache Spark Streaming, and Hazelcast Jet. The results of the study prove the functioning of ESPBench and its toolkit. ESPBench is capable of quantifying performance characteristics of DSPSs and of unveiling differences among systems.
The benchmark proposed in this thesis covers all requirements to be applied in enterprise stream processing settings, and thus represents an improvement over the current state-of-the-art.
The aim of this doctoral thesis was to establish a technique for the analysis of biomolecules with infrared matrix-assisted laser dispersion (IR-MALDI) ion mobility (IM) spectrometry. The main components of the work were the characterization of the IR-MALDI process, the development and characterization of different ion mobility spectrometers, the use of IR-MALDI-IM spectrometry as a robust, standalone spectrometer and the development of a collision cross-section estimation approach for peptides based on molecular dynamics and thermodynamic reweighting.
First, the IR-MALDI source was studied with atmospheric pressure ion mobility spectrometry and shadowgraphy. It consisted of a metal capillary, at the tip of which a self-renewing droplet of analyte solution was met by an IR laser beam. A relationship between peak shape, ion desolvation, diffusion and extraction pulse delay time (pulse delay) was established. First order desolvation kinetics were observed and related to peak broadening by diffusion, both influenced by the pulse delay. The transport mechanisms in IR-MALDI were then studied by relating different laser impact positions on the droplet surface to the corresponding ion mobility spectra. Two different transport mechanisms were determined: phase explosion due to the laser pulse and electrical transport due to delayed ion extraction. The velocity of the ions stemming from the phase explosion was then measured by ion mobility and shadowgraphy at different time scales and distances from the source capillary, showing an initially very high but rapidly decaying velocity. Finally, the anatomy of the dispersion plume was observed in detail with shadowgraphy and general conclusions over the process were drawn.
Understanding the IR-MALDI process enabled the optimization of the different IM spectrometers at atmospheric and reduced pressure (AP and RP, respectively). At reduced pressure, both an AP and an RP IR-MALDI source were used. The influence of the pulsed ion extraction parameters (pulse delay, width and amplitude) on peak shape, resolution and area was systematically studied in both AP and RP IM spectrometers and discussed in the context of the IR-MALDI process. Under RP conditions, the influence of the closing field and of the pressure was also examined for both AP and RP sources. For the AP ionization RP IM spectrometer, the influence of the inlet field (IF) in the source region was also examined. All of these studies led to the determination of the optimal analytical parameters as well as to a better understanding of the initial ion cloud anatomy.
The analytical performance of the spectrometer was then studied. Limits of detection (LOD) and linear ranges were determined under static and pulsed ion injection conditions and interpreted in the context of the IR-MALDI mechanism. Applications in the separation of simple mixtures were also illustrated, demonstrating good isomer separation capabilities and the advantages of singly charged peaks. The possibility to couple high performance liquid chromatography (HPLC) to IR-MALDI-IM spectrometry was also demonstrated. Finally, the reduced pressure spectrometer was used to study the effect of high reduced field strength on the mobility of polyatomic ions in polyatomic gases.
The last focus point was on the study of peptide ions. A dataset obtained with electrospray IM spectrometry was characterized and used for the calibration of a collision cross-section (CCS) determination method based on molecular dynamics (MD) simulations at high temperature. Instead of producing candidate structures which are evaluated one by one, this semi-automated method uses the simulation as a whole to determine a single average collision cross-section value by reweighting the CCS of a few representative structures. The method was compared to the intrinsic size parameter (ISP) method and to experimental results. Additional MD data obtained from the simulations was also used to further analyze the peptides and understand the experimental results, an advantage with regard to the ISP method. Finally, the CCS of peptide ions analyzed by IR-MALDI were also evaluated with both ISP and MD methods and the results compared to experiment, resulting in a first validation of the MD method. Thus, this thesis brings together the soft ionization technique that is IR-MALDI, which produces mostly singly charged peaks, with ion mobility spectrometry, which can distinguish between isomers, and a collision cross-section determination method which also provides structural information on the analyte at hand.