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Electron transfer phenomena in proteins represent one of the most common types of biochemical reactions. They play a central role in energy conversion pathways in living cells, and are crucial components in respiration and photosynthesis. These complex biochemical reaction cascades consist of a series of proteins and protein complexes that couple a charge transfer to different forms of chemical energy. The efficiency and sophisticated optimisation of signal transfer in these natural redox chains has inspired engineering of artificial architectures mimicking essential properties of their natural analogues. Implementation of direct electron transfer (DET) in protein assemblies was a breakthrough in bioelectronics, providing a simple and efficient way for coupling biological recognition events to a signal transducer. DET avoids the use of redox mediators, reducing potential interferences and side reactions, as well as being more compatible with in vivo conditions. However, only a few haem proteins, including the redox protein cytochrome c (cyt.c), and blue copper enzymes show efficient DET on different kinds of electrodes. Previous investigations with cyt.c have mainly focused on heterogeneous electron transfer of monolayers of this protein on gold. An important advance was the fabrication of cyt.c multilayers by electrostatic layer-by-layer self-assembly. The ease of fabrication, the stability, and the controllable permeability of polyelectrolyte multilayers have made them particularly attractive for electroanalytical applications. With cyt.c and sulfonated polyaniline it was for the first time possible that fully electro-active multilayers of the redox protein could be prepared. This approach was extended to design an analytical signal chain based on multilayers of cyt.c and xanthine oxidase (XOD). The system does not need an external mediator but relies on an in situ generation of a mediating radical and thus allows a signal transfer from hypoxanthine via the substrate converting enzyme and cyt.c to the electrode. Another kind of a signal chain is based on assembling proteins in complexes on electrodes in such a way that a direct protein-protein electron transfer becomes feasible. This design does not need a redox mediator in analogy to natural protein communication. For this purpose, cyt.c and the enzyme bilirubin oxidase (BOD, EC 1.3.3.5) are co-immobilized in a self-assembled polyelectrolyte multilayer on gold electrodes. Although these two proteins are not natural reaction partners, the protein architecture facilitates an electron transfer from the electrode via multiple protein layers to molecular oxygen resulting in a significant catalytic reduction current. Finally, we describe a novel strategy for multi-protein layer-by-layer self-assembly combining cyt.c with an enzyme sulfite oxidase (SOx) without use of any additional polymer. Electrostatic interactions between these two proteins with rather separated pI values during the assembly process from a low ionic strength buffer were found sufficient for the layer-by-layer deposition of the both biomolecules. It is anticipated that the concepts described in this work will stimulate further progress in multilayer design of even more complex biomimetic signal cascades taking advantage of direct communication between proteins.
Giacconi et al. (1962) discovered a diffuse cosmic X-ray background with rocket experiments when they searched for lunar X-ray emission. Later satellite missions found a spectral peak in the cosmic X-ray background at ~30 keV. Imaging X-ray satellites such as ROSAT (1990-1999) were able to resolve up to 80% of the background below 2 keV into single point sources, mainly active galaxies. The cosmic X-ray background is the integration of all accreting super-massive (several million solar masses) black holes in the centre of active galaxies over cosmic time. Synthesis models need further populations of X-ray absorbed active galaxy nuclei (AGN) in order to explain the cosmic X-ray background peak at ~30 keV. Current X-ray missions such as XMM-Newton and Chandra offer the possibility of studying these additional populations. This Ph.D. thesis studies the populations that dominate the X-ray sky. For this purpose the 120 ksec XMM-Newton Marano field survey, named for an earlier optical quasar survey in the southern hemisphere, is analysed. Based on the optical follow-up observations the X-ray sources are spectroscopically classified. Optical and X-ray properties of the different X-ray source populations are studied and differences are derived. The amount of absorption in the X-ray spectra of type II AGN, which are considered as a main contributor to the X-ray background at ~30 keV, is determined. In order to extend the sample size of the rare type II AGN, this study also includes objects from another survey, the XMM-Newton Serendipitous Medium Sample. In addition, the dependence of the absorption in type II AGN with redshift and X-ray luminosity is analysed. We detected 328 X-ray sources in the Marano field. 140 sources were spectroscopically classified. We found 89 type I AGN, 36 type II AGN, 6 galaxies, and 9 stars. AGN, galaxies, and stars are clearly distinguishable by their optical and X-ray properties. Type I and II AGN do not separate clearly. They have a significant overlap in all studied properties. In a few cases the X-ray properties are in contradiction to the observed optical properties for type I and type II AGN. For example we find type II AGN that show evidence for optical absorption but are not absorbed in X-rays. Based on the additional use of near infra-red imaging (K-band), we were able to identify several of the rare type II AGN. The X-ray spectra of type II AGN from the XMM-Newton Marano field survey and the XMM-Newton Serendipitous Medium Sample were analysed. Since most of the sources have only ~40 X-ray counts in the XMM-Newton PN-detector, I carefully studied the fit results of simulated X-ray spectra as a function of fit statistic and binning method. The objects revealed only moderate absorption. In particular, I do not find any Compton-thick sources (absorbed by column densities of NH > 1.5 x 10^24 cm^−2). This gives evidence that type II AGN are not the main contributor of the X-ray background around 30 keV. Although bias effects may occur, type II AGN show no noticeable trend of the amount of absorption with redshift or X-ray luminosity.
Im Rahmen der vorliegenden Arbeit ist es erstmals gelungen, mit einem ps-Pumplaser (10 ps) Weißlicht mit einer spektralen Breite von mehr als einer optischen Oktave in einer mikrostrukturierten Faser (MSF) bei einer Pumpwellenlänge von 1064 nm zu generieren. Es ließ sich, abgesehen von nichtkonvertierten Resten der Pumpstrahlung, ein unstrukturiertes und zeitlich stabiles Weißlichtspektrum von 700 nm bis 1650 nm generieren. Die maximale Ausgangsleistung dieser Weißlichtstrahlung betrug 3,1 W. Es konnten sehr gute Einkoppeleffizienzen von maximal 62 % erzielt werden. Die an der Weißlichterzeugung beteiligten dispersiven und nichtlinear optischen Effekte, wie z.B. Selbstphasenmodulation, Vierwellenmischung, Modulationsinstabilitäten oder Solitoneneffekte, werden detailliert theoretisch untersucht und erläutert. Die Arbeit beinhaltet ebenfalls eine umfangreiche Beschreibung der Wirkungsweise und Eigenschaften von mikrostrukturierten Fasern mit einem festen Faserkern. Aufgrund der großen Variationsvielfalt des mikrostrukturierten Fasermantels und der damit verbundenen Wellenleitereigenschaften ergeben sich, insbesondere für die Anwendung in der nichtlinearen Optik, eine Reihe von interessanten Eigenschaften. Es wurden insgesamt vier verschiedene mikrostrukturierte Fasern experimentell untersucht. Für die Interpretation der experimentellen Ergebnisse ist die Pulsausbreitung der ps-Pumppulse in einer dispersiven, nichtlinear optischen Faser anhand der verallgemeinerten nichtlinearen Schrödinger-Gleichung berechnet worden. Durch einen Vergleich der Berechnungen mit den Messdaten ließen sich verstärkte Modulationsinstabilitäten und verschiedene Solitoneneffekte als hauptsächlich für die Weißlichterzeugung bei ps-Anregungspulsen verantwortlich identifizieren. Auf der Basis der durchgeführten Untersuchungen wurde in Kooperation mit der Fa. Jenoptik Laser, Optik, Systeme GmbH eine kompakte und leistungsstarke Weißlichtquelle entwickelt. Diese wurde erfolgreich in einer Kohärenztomographiemessung (Optical Coherence Tomography - OCT) getestet: Es konnte in ex vivo-Untersuchungen gezeigt werden, dass sich mit dieser ps-Weißlichtquelle eine hohe Eindringtiefe von ca. 400 µm in die Netzhaut eines Affen erreichen lässt.
In dieser Arbeit wurde die Variabilität der Atmosphäre in einem neuen gekoppelten Klimamodell (ECHO-GiSP) untersucht, welches eine vereinfachte Stratosphärenchemie (bis 80 km Höhe) enthält. Es wurden 2 Simulationen über 150 Jahre durchgeführt. In einer der Simulationen wurde die atmosphärische Chemie modelliert, hatte aber keinen Einfluß auf die Dynamik des Klimamodelles. In der zweiten Simulation wurde hingegen die Wirkung der Chemie auf die Klimadynamik explizit berücksichtigt, die über die Strahlungsbilanz des Modelles erfolgt. Dies ist die erste Langzeitsimulation mit einem voll gekoppelten globalen Klimamodell mit interaktiver Chemie. Die Simulation mit rückgekoppelter Chemie zeigt eine Abschwächung des atmosphärischen Variabilitätsmusters der Arktischen Oszillation (AO). Zudem kommt es in der Troposphäre zu einer Reduzierung der mittleren Windgeschwindigkeiten der gemäßigten Breiten aufgrund verringerter Temperaturgegensätze zwischen den Tropen und den Polargebieten. Auch in der Stratosphäre ergibt sich eine Abschwächung und Erwärmung des Polarwirbels. Diese Auswirkungen der Kopplung zwischen der atmosphärischen Chemie und der Dynamik des Klimamodelles sind eine wichtige Erkenntnis, da in früheren Klimasimulationen die Variabilität der AO oft zu stark ausgeprägt war. In der Stratosphäre reduziert sich infolge des abgeschwächten Polarwirbels auch die großräumige Zirkulation zwischen den beiden Hemisphären der Erde. In der Troposphäre werden hingegen die allgemeine Zirkulation, und damit auch die subtropischen Strahlströme des Windes verstärkt. Zudem kommt es in den Tropen zu Temperaturänderungen durch stratosphärische Ozonschwankungen in Abhängigkeit von der AO. Allgemein verändert sich die Kopplung zwischen Troposphäre und Stratosphäre, einschließlich des durch die Anregung von langen atmosphärischen Wellen erfolgenden vertikalen Energieübertrages aus der Troposphäre in die Stratosphäre.
In this work, some new results to exploit the recurrence properties of quasiperiodic dynamical systems are presented by means of a two dimensional visualization technique, Recurrence Plots(RPs). Quasiperiodicity is the simplest form of dynamics exhibiting nontrivial recurrences, which are common in many nonlinear systems. The concept of recurrence was introduced to study the restricted three body problem and it is very useful for the characterization of nonlinear systems. I have analyzed in detail the recurrence patterns of systems with quasiperiodic dynamics both analytically and numerically. Based on a theoretical analysis, I have proposed a new procedure to distinguish quasiperiodic dynamics from chaos. This algorithm is particular useful in the analysis of short time series. Furthermore, this approach demonstrates to be efficient in recognizing regular and chaotic trajectories of dynamical systems with mixed phase space. Regarding the application to real situations, I have shown the capability and validity of this method by analyzing time series from fluid experiments.
In der vorliegenden Arbeit werden Methoden der Erdsystemanalyse auf die Untersuchung der Habitabilität terrestrischer Exoplaneten angewandt. Mit Hilfe eines parametrisierten Konvektionsmodells für die Erde wird die thermische Evolution von terrestrischen Planeten berechnet. Bei zunehmender Leuchtkraft des Zentralsterns wird über den globalen Karbonat-Silikat-Kreislauf das planetare Klima stabilisiert. Für eine photosynthetisch-aktive Biosphäre, die in einem bestimmten Temperaturbereich bei hinreichender CO2-Konzentration existieren kann, wird eine Überlebenspanne abgeschätzt. Der Abstandsbereich um einen Stern, in dem eine solche Biosphäre produktiv ist, wird als photosynthetisch-aktive habitable Zone (pHZ) definiert und berechnet. Der Zeitpunkt, zu dem die pHZ in einem extrasolaren Planetensystem endgültig verschwindet, ist die maximale Lebenspanne der Biosphäre. Für Supererden, massereiche terrestrische Planeten, ist sie umso länger, je massereicher der Planet ist und umso kürzer, je mehr er mit Kontinenten bedeckt ist. Für Supererden, die keine ausgeprägten Wasser- oder Landwelten sind, skaliert die maximale Lebenspanne mit der Planetenmasse mit einem Exponenten von 0,14. Um K- und M-Sterne ist die Überlebensspanne einer Biosphäre auf einem Planeten immer durch die maximale Lebensspanne bestimmt und nicht durch das Ende der Hauptreihenentwicklung des Zentralsterns limitiert. Das pHZ-Konzept wird auf das extrasolare Planetensystem Gliese 581 angewandt. Danach könnte die 8-Erdmassen-Supererde Gliese 581d habitabel sein. Basierend auf dem vorgestellten pHZ-Konzept wird erstmals die von Ward und Brownlee 1999 aufgestellte Rare-Earth-Hypothese für die Milchstraße quantifiziert. Diese Hypothese besagt, dass komplexes Leben im Universum vermutlich sehr selten ist, wohingegen primitives Leben weit verbreitet sein könnte. Unterschiedliche Temperatur- und CO2-Toleranzen sowie ein unterschiedlicher Einfluss auf die Verwitterung für komplexe und primitive Lebensformen führt zu unterschiedlichen Grenzen der pHZ und zu einer unterschiedlichen Abschätzung für die Anzahl der Planeten, die mit den entsprechenden Lebensformen besiedelt sein könnten. Dabei ergibt sich, dass komplex besiedelte Planeten heute etwa 100-mal seltener sein müssten als primitiv besiedelte.
The biological function and the technological applications of semiflexible polymers, such as DNA, actin filaments and carbon nanotubes, strongly depend on their rigidity. Semiflexible polymers are characterized by their persistence length, the definition of which is the subject of the first part of this thesis. Attractive interactions, that arise e.g.~in the adsorption, the condensation and the bundling of filaments, can change the conformation of a semiflexible polymer. The conformation depends on the relative magnitude of the material parameters and can be influenced by them in a systematic manner. In particular, the morphologies of semiflexible polymer rings, such as circular nanotubes or DNA, which are adsorbed onto substrates with three types of structures, are studied: (i) A topographical channel, (ii) a chemically modified stripe and (iii) a periodic pattern of topographical steps. The results are compared with the condensation of rings by attractive interactions. Furthermore, the bundling of two individual actin filaments, whose ends are anchored, is analyzed. This system geometry is shown to provide a systematic and quantitative method to extract the magnitude of the attraction between the filaments from experimentally observable conformations of the filaments.
The role played by azobenzene polymers in the modern photonic, electronic and opto-mechanical applications cannot be underestimated. These polymers are successfully used to produce alignment layers for liquid crystalline fluorescent polymers in the display and semiconductor technology, to build waveguides and waveguide couplers, as data storage media and as labels in quality product protection. A very hot topic in modern research are light-driven artificial muscles based on azobenzene elastomers. The incorporation of azobenzene chromophores into polymer systems via covalent bonding or even by blending gives rise to a number of unusual effects under visible (VIS) and ultraviolet light irradiation. The most amazing effect is the inscription of surface relief gratings (SRGs) onto thin azobenzene polymer films. At least seven models have been proposed to explain the origin of the inscribing force but none of them describes satisfactorily the light induced material transport on the molecular level. In most models, to explain the mass transport over micrometer distances during irradiation at room temperature, it is necessary to assume a considerable degree of photoinduced softening, at least comparable with that at the glass transition. Contrary to this assumption, we have gathered a convincing evidence that there is no considerable softening of the azobenzene layers under illumination. Presently we can surely say that light induced softening is a very weak accompanying effect rather than a necessary condition for the formation of SRGs. This means that the inscribing force should be above the yield point of the azobenzene polymer. Hence, an appropriate approach to describe the formation and relaxation of SRGs is a viscoplastic theory. It was used to reproduce pulse-like inscription of SRGs as measured by VIS light scattering. At longer inscription times the VIS scattering pattern exhibits some peculiarities which can be explained by the appearance of a density grating that will be shown to arise due to the final compressibility of the polymer film. As a logical consequence of the aforementioned research, a thermodynamic theory explaining the light-induced deformation of free standing films and the formation of SRGs is proposed. The basic idea of this theory is that under homogeneous illumination an initially isotropic sample should stretch itself along the polarization direction to compensate the entropy decrease produced by the photoinduced reorientation of azobenzene chromophores. Finally, some ideas about further development of this controversial topic will be discussed.
Magnetorotational instability (MRI) is one of the most important and most common instabilities in astrophysics. Today it is widely accepted that it serves as a major source of turbulent viscosity in accretion disks, the most energy efficient objects in the universe. The importance of the MRI for astrophysics has been realized only in recent fifteen years. However, originally it was discovered much earlier, in 1959, in a very different context. Theoretical flow of a conducting liquid confined between differentially rotating cylinders in the presence of an external magnetic field was analyzed. The central conclusion is that the additional magnetic field parallel to the axis of rotation can destabilize otherwise stable flow. Theory of non-magnetized fluid motion between rotating cylinders has much longer history, though. It has been studied already in 1888 and today such setup is usually referred as a Taylor-Couette flow. To prove experimentally the existence of MRI in a magnetized Taylor-Couette flow is a demanding task and different MHD groups around the world try to achieve it. The main problem lies in the fact that laboratory liquid metals which are used in such experiments are characterized by small magnetic Prandtl number. Consequently rotation rates of the cylinders must be extremely large and vast amount of technical problems emerge. One of the most important difficulties is an influence of plates enclosing the cylinders in any experiment. For fast rotation the plates tend to dominate the whole flow and the MRI can not be observed. In this thesis we discuss a special helical configuration of the applied magnetic field which allows the critical rotation rates to be much smaller. If only the axial magnetic field is present, the cylinders must rotate with angular velocities corresponding to Reynolds numbers of order Re ≈ 10^6. With the helical field this number is dramatically reduced to Re ≈ 10^3. The azimuthal component of the magnetic field can be easily generated by letting an electric current through the axis of rotation, In a Taylor-Couette flow the (primary) instability manifests itself as Taylor vortices. The specific geometry of the helical magnetic field leads to a traveling wave solution and the vortices are drifting in a direction determined by rotation and the magnetic field. In an idealized study for infinitely long cylinders this is not a problem. However, if the cylinders have finite length and are bounded vertically by the plates the situation is different. In this dissertation it is shown, with use of numerical methods, that the traveling wave solution also exists for MHD Taylor-Couette flow at finite aspect ratio H/D, H being height of the cylinders, D width of the gap between them. The nonlinear simulations provide amplitudes of fluid velocity which are helpful in designing an experiment. Although the plates disturb the flow, parameters like the drift velocity indicate that the helical MRI operates in this case. The idea of the helical MRI was implemented in a very recent experiment PROMISE. The results provided, for the first time, an evidence that the (helical) MRI indeed exists. Nevertheless, the influence of the vertical endplates was evident and the experiment can be, in principle, improved. Exemplary methods of reduction of the end-effect are here proposed. Near the vertical boundaries develops an Ekman-Hartmann layer. Study of this layer for the MHD Taylor-Couette system as well as its impact on the global flow properties is presented. It is shown that the plates, especially if they are conducting, can disturb the flow far more then previously thought also for relatively slow rotation rates.
This work is concerned with the spatio-temporal structures that emerge when non-identical, diffusively coupled oscillators synchronize. It contains analytical results and their confirmation through extensive computer simulations. We use the Kuramoto model which reduces general oscillatory systems to phase dynamics. The symmetry of the coupling plays an important role for the formation of patterns. We have studied the ordering influence of an asymmetry (non-isochronicity) in the phase coupling function on the phase profile in synchronization and the intricate interplay between this asymmetry and the frequency heterogeneity in the system. The thesis is divided into three main parts. Chapter 2 and 3 introduce the basic model of Kuramoto and conditions for stable synchronization. In Chapter 4 we characterize the phase profiles in synchronization for various special cases and in an exponential approximation of the phase coupling function, which allows for an analytical treatment. Finally, in the third part (Chapter 5) we study the influence of non-isochronicity on the synchronization frequency in continuous, reaction diffusion systems and discrete networks of oscillators.