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Microswimmers, i.e. swimmers of micron size experiencing low Reynolds numbers, have received a great deal of attention in the last years, since many applications are envisioned in medicine and bioremediation. A promising field is the one of magnetic swimmers, since magnetism is biocom-patible and could be used to direct or actuate the swimmers. This thesis studies two examples of magnetic microswimmers from a physics point of view.
The first system to be studied are magnetic cells, which can be magnetic biohybrids (a swimming cell coupled with a magnetic synthetic component) or magnetotactic bacteria (naturally occurring bacteria that produce an intracellular chain of magnetic crystals). A magnetic cell can passively interact with external magnetic fields, which can be used for direction. The aim of the thesis is to understand how magnetic cells couple this magnetic interaction to their swimming strategies, mainly how they combine it with chemotaxis (the ability to sense external gradient of chemical species and to bias their walk on these gradients). In particular, one open question addresses the advantage given by these magnetic interactions for the magnetotactic bacteria in a natural environment, such as porous sediments. In the thesis, a modified Active Brownian Particle model is used to perform simulations and to reproduce experimental data for different systems such as bacteria swimming in the bulk, in a capillary or in confined geometries. I will show that magnetic fields speed up chemotaxis under special conditions, depending on parameters such as their swimming strategy (run-and-tumble or run-and-reverse), aerotactic strategy (axial or polar), and magnetic fields (intensities and orientations), but it can also hinder bacterial chemotaxis depending on the system.
The second example of magnetic microswimmer are rigid magnetic propellers such as helices or random-shaped propellers. These propellers are actuated and directed by an external rotating magnetic field. One open question is how shape and magnetic properties influence the propeller behavior; the goal of this research field is to design the best propeller for a given situation. The aim of the thesis is to propose a simulation method to reproduce the behavior of experimentally-realized propellers and to determine their magnetic properties. The hydrodynamic simulations are based on the use of the mobility matrix. As main result, I propose a method to match the experimental data, while showing that not only shape but also the magnetic properties influence the propellers swimming characteristics.
This project was focused on exploring the phase behavior of poly(styrene)187000-block-poly(2-vinylpyridine)203000 (SV390) with high molecular weight (390 kg/mol) in thin films, in which the self-assembly of block copolymers (BCPs) was realized via thermo-solvent annealing. The advanced processing technique of solvent vapor treatment provides controlled and stable conditions.
In Chapter 3, the factors to influence the annealing process and the swelling behavior of homopolymers are presented and discussed. The swelling behavior of BCP in films is controlled by the temperature of the vapor and of the substrate, on one hand, and variation of the saturation of the solvent vapor atmosphere (different solvents), on the other hand. Additional factors like the geometry and material of the chamber, the type of flow inside the chamber etc. also influence the reproducibility and stability of the processing. The slightly selective solvent vapor of chloroform gives 10% more swelling of P2VP than PS in films with thickness of ~40 nm.
The tunable morphology in ultrathin films of high molecular weight BCP (SV390) was investigated in Chapter 4. First, the swelling behavior can be precisely tuned by temperature and/or vapor flow separately, which provided information for exploring the multiple-parameter-influenced segmental chain mobility of polymer films. The equilibrium state of SV390 in thin films influenced by temperature was realized at various temperatures with the same degree of swelling. Various methods including characterization with SFM, metallization and RIE were used to identify the morphology of films as porous half-layer with PS dots and P2VP matrix. The kinetic investigations demonstrate that on substrates with either weak or strong interaction the original morphology of the BCP with high molecular weight is changed very fast within 5 min, and the further annealing serves for annihilation of defects.
The morphological development of symmetric BCP in films with thickness increasing from half-layer to one-layer influenced by confinement factors of gradient film thicknesses and various surface properties of substrates was studied in Chapter 5. SV390 and SV99 films show bulk lamella-forming morphology after slightly selective solvent vapor (chloroform) treatment. SV99 films show cylinder-forming morphology under strongly selective solvent vapor (toluene) treatment since the asymmetric structure (caused by toluene uptake in PS blocks only) of SV99 block copolymer during annealing. Both kinds of morphology (lamella and cylinder) are influenced by the film thickness. The annealed morphology of SV390 and SV99 influenced by the combination of confined film and substrate property is similar to the morphology on flat silicon wafers. In this chapter the gradients in the film thickness and surface properties of the substrates with regard to their influence on the morphological development in thin BCP films are presented. Directed self-assembly (graphoepitaxy) of this SV390 was also investigated to compare with systematically reported SV99.
In Chapter 6 an approach to induced oriented microphase separation in thick block copolymer films via treatment with the oriented vapor flow using mini-extruder is envisaged to be an alternative to existing methodologies, e.g. via non-solvent-induced phase separation. The preliminary tests performed in this study confirm potential perspective of this method, which alters the structure through the bulk of the film (as revealed by SAXS measurements), but more detailed studies have to be conducted in order to optimize the preparation.
BACKGROUND: Physical activity involving high spinal load has been exposed to possess a crucial impact in the genesis of acute and chronic low back pain and disorder. Vigorous spinal loads are surmised in drop landings, for which strenuous bending loads were formerly evinced for the lower extremity structures. Thus far, clinical studies revealed that repetitive landing impacts can evoke benign structural adaptions or damage to the lumbar vertebrae. Though, causes for these observations are hitherto not conclusively evinced; since actual spinal load has to date not been experimentally documented. Moreover, it is yet undetermined how physiological activation of trunk musculature compensates for landing impact induced spinal loads, and to which extend trunk activity and spinal load are affected by landing demands and performer characteristics. AIMS of this study are 1. the localisation and quantification of spinal bending loads under various landing demands and 2. the identification of compensatory trunk muscular activity pattern, which potentially alleviate spinal load magnitudes. Three consecutive Hypotheses (H1 - H3) were hereto postulated: H1 posits that spinal bending loads in segregated motion planes can feasibly and reliably be evaluated from peak spine segmental angular accelerations. H2 furthermore assumes that vertical drop landings elicit highest spine bending load in sagittal flexion of the lumbar spine. Based on these verifications, a second study shall prove the successive hypothesis (H3) that diversified landing conditions, like performer’s landing familiarity and gender, as an implementation of an instantaneous follow-up task, affect the emerging lumbar spinal bending load. Herein it is moreover surmised that lumbar spinal bending loads under distinct landing conditions are predominantly modulated by herewith disparately deployed conditioned pre-activations of trunk muscles. METHODS: To test the above arrayed hypothesis, two successive studies were carried out. In STUDY 1, 17 subjects were repetitively assessed performing various drop landings (heigth: 15, 30, 45, 60cm; unilateral, bilateral, blindfolded, catching a ball) in a test-retest-design. Herein individual peak angular accelerations [αMAX] were derived from three-dimensional motion data of four trunk-segments (upper thoracic, lower thoracic, lumbar, pelvis). αMAX was herein assessed in flexion, lateral flexion, and rotation of each spinal joint, formed by two adjacent segments. Reliability of αMAX within and between test-days was evaluated by CV%, ICC 2.1, TRV%, and Bland & Altman Analysis (BIAS±LoA). Subsequently, peak flexion acceleration of the lumbo-pelvic joint [αFLEX[LS-PV]] was statistically compared to αMAX expressions of each other assessed spinal joint and motion plane (Mean ±SD, Independent Samples T-test). STUDY 2 deliberately assessed mere peak lumbo-pelvic flexion accelerations [αFLEX[LS-PV]] and electro-myographic trunk pre-activity prior to αFLEX[LS-PV] on 43 subjects performing varied landing tasks (height 45cm; with definite or indefinite predictability of a subsequent instant follow up jump). Subjects were contrasted with respect to their previous landing familiarity ( >1000 vs. <100 landings performed in the past 10 years) and gender. Differences of αFLEX[LS-PV] and muscular pre-activity between contrasted subject groups as between landing tasks were equally statistically tested by three-way mixed ANOVA with Post-hoc tests. Associations between αFLEX[LS-PV] and muscular pre-activity were factor-specifically assessed by Spearman’s rank order correlation coefficient (rS). Complementarily, muscular pre-activity was subdivided by landing phases [DROP, IMPACT] and discretely assessed for phase specific associations to αFLEX[LS-PV]. Each muscular activity was moreover pairwise compared between DROP and IMPACT (Mean ±SD, Dependent Samples T-test). RESULTS: αMAX was presented with overall high variability within test-days (CV =36%). Lowest intra-individual variability and highest reproducibility of αMAX between test-days was shown in flexion of the spine. αFLEX[LS-PV] showed largely consistent sig. higher magnitudes compared to αMAX presented in more cranial spinal joints and other motion planes. αFLEX[LS-PV] moreover gradually increased with escalations in landing heights. Landing unfamiliar subjects presented sig. higher αFLEX[LS-PV] in contrast to landing familiar ones (p=.016). M. Obliquus Int. with M. Transversus Abd. (66 ±32%MVC) and M. Erector Spinae (47 ±15%MVC) presented maredly highest activity in contrast to lowest activity of M. Rectus Abd. (10 ±4%MVC). Landing unfamiliar subjects showed compared to landing familiar ones sig. higher activity of M. Obliquus Ext. (17 ±8%MVC, 12 ±7%MVC, p= .044). M. Obliquus Ext. and its co-contraction ratio with M. Erector Spinae moreover exhibited low but sig. positive correlations to αFLEX[LS-PV] (rs=.39, rs=.31). Each trunk muscule distributed larger shares of its activity to DROP, whereas peak activations of most muscles emerged in the proportionally shorter IMPACT phase. Commonly increased muscular pre-activation particularly at IMPACT was found in landings with a contrived follow up jump and in female subjects, whereby αFLEX[LS-PV] was hereof only marginally affected. DISCUSSION: Highest spine segmental angular accelerations in drop landings emerge in sagittal flexion of the lumbar spine. The compensatory stabilisation of the spine appears to be preponderantly provided by a dorso-ventral co-contraction of M. Obliquus Int., M. Transversus Abd. and M. Erector Spinae. Elevated pre-activity of M. Obliquuis Ext. supposably characterises poor landing experience, which might engender increased bending loads to the lumbar spine. A pervasive large variability of spinal angular accelerations measured across all landing types, suggests a multifarious utilisation of diverse mechanisms compensating for spinal impacts in landing performances. A standardised assessment and valid evaluation of landing evoked lumbar bending loads is hereof largley confined. CONCLUSION: Drop landings elicit most strenuous lumbo-pelvic flexion accelerations, which can be appraised as representatives for high energetic bending loads to the spine. Such entail the highest risk to overload the spinal tissue, when landing demands exceed the individual’s landing skill. Previous landing experience and training appears to effectively improve muscular spine stabilisation pattern, diminishing spinal bending loads.
East Africa is a natural laboratory: Studying its unique geological and biological history can help us better inform our theories and models. Studying its present and future can help us protect its globally important biodiversity and ecosystem services. East African vegetation plays a central role in all these aspects, and this dissertation aims to quantify its dynamics through computer simulations.
Computer models help us recreate past settings, forecast into the future or conduct simulation experiments that we cannot otherwise perform in the field. But before all that, one needs to test their performance. The outputs that the model produced using the present day-inputs, agreed well with present-day observations of East African vegetation. Next, I simulated past vegetation for which we have fossil pollen data to compare. With computer models, we can fill the gaps of knowledge between sites where we have fossil pollen data from, and create a more complete picture of the past. Good level of agreement between model and pollen data where they overlapped in space further validated our model performance.
Once the model was tested and validated for the region, it became possible to probe one of the long standing questions regarding East African vegetation: How did East Africa lose its tropical forests? The present-day vegetation in the tropics is mainly characterized by continuous forests worldwide except in tropical East Africa, where forests only occur as patches. In a series of simulation experiments, I was able to show under which conditions these forest patches could have been connected and fragmented in the past. This study showed the sensitivity of East African vegetation to climate change and variability such as those expected under future climate change.
El Niño Southern Oscillation (ENSO) events that result from the fluctuations in temperature between the ocean and atmosphere, bring further variability to East African climate and are predicted to increase in intensity in the future. But climate models are still not good at capturing the pattens of these events. In a study where I quantified the influence of ENSO events on East African vegetation, I showed how different the future vegetation could be from what we currently predict with these climate models that lack accurate ENSO contribution. Consideration of these discrepancies is important for our future global carbon budget calculations and management decisions.
Ferroic materials have attracted a lot of attention over the years due to their wide range of applications in sensors, actuators, and memory devices. Their technological applications originate from their unique properties such as ferroelectricity and piezoelectricity. In order to optimize these materials, it is necessary to understand the coupling between their nanoscale structure and transient response, which are related to the atomic structure of the unit cell.
In this thesis, synchrotron X-ray diffraction is used to investigate the structure of ferroelectric thin film capacitors during application of a periodic electric field. Combining electrical measurements with time-resolved X-ray diffraction on a working device allows for visualization of the interplay between charge flow and structural motion. This constitutes the core of this work. The first part of this thesis discusses the electrical and structural dynamics of a ferroelectric Pt/Pb(Zr0.2,Ti0.8)O3/SrRuO3 heterostructure during charging, discharging, and polarization reversal. After polarization reversal a non-linear piezoelectric response develops on a much longer time scale than the RC time constant of the device. The reversal process is inhomogeneous and induces a transient disordered domain state. The structural dynamics under sub-coercive field conditions show that this disordered domain state can be remanent and can be erased with an appropriate voltage pulse sequence. The frequency-dependent dynamic characterization of a Pb(Zr0.52,Ti0.48)O3 layer, at the morphotropic phase boundary, shows that at high frequency, the limited domain wall velocity causes a phase lag between the applied field and both the structural and electrical responses. An external modification of the RC time constant of the measurement delays the switching current and widens the electromechanical hysteresis loop while achieving a higher compressive piezoelectric strain within the crystal.
In the second part of this thesis, time-resolved reciprocal space maps of multiferroic BiFeO3 thin films were measured to identify the domain structure and investigate the development of an inhomogeneous piezoelectric response during the polarization reversal. The presence of 109° domains is evidenced by the splitting of the Bragg peak.
The last part of this work investigates the effect of an optically excited ultrafast strain or heat pulse propagating through a ferroelectric BaTiO3 layer, where we observed an additional current response due to the laser pulse excitation of the metallic bottom electrode of the heterostructure.
Synthesis of artificial building blocks for sortase-mediated ligation and their enzymatic linkage
(2018)
The enzyme Sortase A catalyzes the formation of a peptide bond between the recognition sequence LPXTG and an oligoglycine. While manifold ligations between proteins and various biomolecules, proteins and small synthetic molecules as well as proteins and surfaces have been reported, the aim of this thesis was to investigate the sortase-catalyzed linkage between artificial building blocks. Hence, this could pave the way for the use of sortase A for tasks from a chemical point of view and maybe even materials science.
For the proof of concept, the studied systems were kept as simple as possible at first by choosing easily accessible silica NPs and commercially available polymers. These building blocks were functionalized with peptide motifs for sortase-mediated ligation. Silica nanoparticles were synthesized with diameters of 60 and 200 nm and surface modified with C=C functionalities. Then, peptides bearing a terminal cysteine were covalently linked by means of a thiol-ene reaction. 60 nm SiO2 NPs were functionalized with pentaglycines, while peptides with LPETG motif were linked to 200 nm silica particles. Polyethyleneglycol (PEG) and poly(N isopropylacrylamide) (PNIPAM) were likewise functionalized with peptides by thiol-ene reaction between cysteine residues and C=C units in the polymer end groups. Hence, G5-PEG and PNIPAM-LPETG conjugates were obtained. With this set of building blocks, NP–polymer hybrids, NP–NP, and polymer–polymer structures were generated by sortase-mediated ligation and the product formation shown by transmission electron microscopy, MALDI-ToF mass spectrometry and dynamic light scatting, among others. Thus, the linkage of these artificial building blocks by the enzyme sortase A could be demonstrated.
However, when using commercially available polymers, the purification of the polymer–peptide conjugates was impossible and resulted in a mixture containing unmodified polymer. Therefore, strategies were developed for the own synthesis of pure peptide-polymer and polymer-peptide conjugates as building blocks for sortase-mediated ligation. The designed routes are based on preparing polymer blocks via RAFT polymerization from CTAs that are attached to N- or C-terminus, respectively, of a peptide. GG-PNIPAM was synthesized through attachment of a suitable RAFT CTA to Fmoc-GG in an esterification reaction, followed by polymerization of NIPAM and cleavage of the Fmoc protection group. Furthermore, several peptides were synthesized by solid-phase peptide synthesis. The linkage of a RAFT CTA (or
polymerization initiator) to the N-terminus of a peptide can be conducted in an automated fashion as last step in a peptide synthesizer. The synthesis of such a conjugate couldn’t be realized in the time frame of this thesis, but many promising strategies exist to continue this strategy using different coupling reagents. Such polymer building blocks can be used to synthesize protein-polymer conjugates catalyzed by sortase A and the approach can be carried on to the synthesis of block copolymers by using polymer blocks with peptide motifs on both ends.
Although the proof of concept demonstrated in this thesis only shows examples that can be also synthesized by exclusively chemical techniques, a toolbox of such building blocks will enable the future formation of new materials and pave the way for the application of enzymes in materials science. In addition to nanoparticle systems and block copolymers, this also includes combination with protein-based building blocks to form hybrid materials. Hence, sortase could become an enzymatic tool that complements established chemical linking technologies and provides specific peptide motifs that are orthogonal to all existing chemical functional groups.
Thematic role assignment and word order preferences in the child language acquisition of Tagalog
(2018)
A critical task in daily communications is identifying who did what to whom in an utterance, or assigning the thematic roles agent and patient in a sentence. This dissertation is concerned with Tagalog-speaking children’s use of word order and morphosyntactic markers for thematic role assignment. It aims to explain children’s difficulties in interpreting sentences with a non-canonical order of arguments (i.e., patient-before-agent) by testing the predictions of the following accounts: the frequency account (Demuth, 1989), the Competition model (MacWhinney & Bates, 1989), and the incremental processing account (Trueswell & Gleitman, 2004). Moreover, the experiments in this dissertation test the influence of a word order strategy in a language like Tagalog, where the thematic roles are always unambiguous in a sentence, due to its verb-initial order and its voice-marking system. In Tagalog’s voice-marking system, the inflection on the verb indicates the thematic role of the noun marked by 'ang.' First, the possible basis for a word order strategy in Tagalog was established using a sentence completion experiment given to adults and 5- and 7-year-old children (Chapter 2) and a child-directed speech corpus analysis (Chapter 3). In general, adults and children showed an agent-before-patient preference, although adults’ preference was also affected by sentence voice. Children’s comprehension was then examined through a self-paced listening and picture verification task (Chapter 3) and an eye-tracking and picture selection task (Chapter 4), where word order (agent-initial or patient-initial) and voice (agent voice or patient voice) were manipulated. Offline (i.e., accuracy) and online (i.e., listening times, looks to the target) measures revealed that 5- and 7-year-old Tagalog-speaking children had a bias to interpret the first noun as the agent. Additionally, the use of word order and morphosyntactic markers was found to be modulated by voice. In the agent voice, children relied more on a word order strategy; while in the patient voice, they relied on the morphosyntactic markers. These results are only partially explained by the accounts being tested in this dissertation. Instead, the findings support computational accounts of incremental word prediction and learning such as Chang, Dell, & Bock’s (2006) model.
Future magnetic recording industry needs a high-density data storage technology. However, switching the magnetization of small bits requires high magnetic fields that cause excessive heat dissipation. Therefore, controlling magnetism without applying external magnetic field is an important research topic for potential applications in data storage devices with low power consumption. Among the different approaches being investigated, two of them stand out, namely i) all-optical helicity dependent switching (AO-HDS) and ii) ferroelectric control of magnetism. This thesis aims to contribute towards a better understanding of the physical processes behinds these effects as well as reporting new and exciting possibility for the optical and/or electric control of magnetic properties. Hence, the thesis contains two differentiated chapters of results; the first devoted to AO-HDS on TbFe alloys and the second to the electric field control of magnetism in an archetypal Fe/BaTiO3 system.
In the first part, the scalability of the AO-HDS to small laser spot-sizes of few microns in the ferrimagnetic TbFe alloy is investigated by spatially resolving the magnetic contrast with photo-emission electron microscopy (PEEM) and X-ray magnetic circular dichroism (XMCD). The results show that the AO-HDS is a local effect within the laser spot size that occurs in the ring-shaped region in the vicinity of thermal demagnetization. Within the ring region, the helicity dependent switching occurs via thermally activated domain wall motion. Further, the thesis reports on a novel effect of thickness dependent inversion of the switching orientation. It addresses some of the important questions like the role of laser heating and the microscopic mechanism driving AO-HDS.
The second part of the thesis focuses on the electric field control of magnetism in an artificial multiferroic heterostructure. The sample consists of an Fe wedge with thickness varying between 0:5 nm and 3 nm, deposited on top of a ferroelectric and ferroelastic BaTiO3 [001]-oriented single crystal substrate. Here, the magnetic contrast is imaged via PEEM and XMCD as a function of out-of-plane voltage. The results show the evidence of the electric field control of superparamagnetism mediated by a ferroelastic modification of the magnetic anisotropy. The changes in the magnetoelastic anisotropy drive the transition from the superparamagnetic to superferromagnetic state at localized sample positions.
Various ways of preparing enantiomerically pure 2-amino[6]helicene derivatives were explored. Ni(0) mediated cyclotrimerization of enantiopure triynes provided (M)- and (P)-7,8-bis(p-tolyl)hexahelicene-2-amine in >99% ee as well as its benzoderivative in >99% ee. The stereocontrol was found to be inefficient for a 2- aminobenzo[6]helicene congener with an embedded five-membered ring. Helically chiral imidazolium salts bearing one or two helicene moieties have been synthesized and applied in enantioselective [2+2+2] cyclotrimerization catalyzed by an in situ formed Ni(0)-NHC complex. The synthesis of the first helically chiral Pd- and Ru-NHC complexes and their application in enantioselective catalysis was demonstrated. The latter shows promising results in enantioselective olefin metathesis reactions. A mechanistic proposal for asymmetric ring closing metathesis is provided.
Eta Carinae
(2018)
The exceptional binary star Eta Carinae has been fascinating scientists and the people in the Southern hemisphere alike for hundreds of years. It survived an enormous outbreak, comparable to a supernova energy-wise, and for a short period became the brightest star of the night sky. From observations from the radio regime to X-rays the system's characteristics and its emission in photon energies up to ~ 50 keV are well studied today. The binary is composed of two massive stars of ~ 30 and ~ 100 solar masses. Either star drives a strong stellar wind that continuously carries away a fraction of its mass. The collision of these winds leads to a shock on each side of the encounter. In the wind-wind-collision region plasma gets heated when it is overrun by the shocks. Part of the emission seen in X-rays can be attributed to this plasma. Above ~ 50 keV the emission is no longer of thermal origin: the required plasma temperature exceeds the available mechanical energy input of the stellar winds. In contrast to its observational history in thermal energies observational evidence of Eta Carinae's non-thermal emission has only recently built up. In high-energy gamma-rays Eta Carinae is the only binary of its kind that has been detected unambiguously. Its energy spectrum reaches up to ~ hundred GeV, a regime where satellite-based gamma-ray experiments run out of statistics. Ground-based gamma-ray experiments have the advantage of large photon collection areas. H.E.S.S. is the only gamma-ray experiment located in the Southern hemisphere and thus able to observe Eta Carinae in this energy range. H.E.S.S. measures gamma-rays via electromagnetic showers of particles that very-high-energy gamma-rays initiate in the atmosphere. The main challenge in observations of Eta Carinae with H.E.S.S. is the UV emission of the Carina nebula that leads to a background that is up to 10 times stronger than usual for H.E.S.S. This thesis presents the first detection of a colliding-wind binary in very-high-energy gamma-rays and documents the studies that led to it. The differential gamma-ray energy spectrum of Eta Carinae is measured up to 700 GeV. A hadronic and leptonic origin of the gamma-ray emission is discussed and based on the comparison of cooling times a hadronic scenario is favoured.