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Context. Over the past 20 yr, the quietest areas of the solar surface have revealed a weak but extremely dynamic magnetism occurring at small scales (<500 km), which may provide an important contribution to the dynamics and energetics of the outer layers of the atmosphere. Understanding this magnetism requires the inference of physical quantities from high-sensitivity spectro-polarimetric data with high spatio-temporal resolution. Aims. We present high-precision spectro-polarimetric data with high spatial resolution (0.4") of the very quiet Sun at 1.56 mu m obtained with the GREGOR telescope to shed some light on this complex magnetism. Methods. We used inversion techniques in two main approaches. First, we assumed that the observed profiles can be reproduced with a constant magnetic field atmosphere embedded in a field-free medium. Second, we assumed that the resolution element has a substructure with either two constant magnetic atmospheres or a single magnetic atmosphere with gradients of the physical quantities along the optical depth, both coexisting with a global stray-light component. Results. Half of our observed quiet-Sun region is better explained by magnetic substructure within the resolution element. However, we cannot distinguish whether this substructure comes from gradients of the physical parameters along the line of sight or from horizontal gradients (across the surface). In these pixels, a model with two magnetic components is preferred, and we find two distinct magnetic field populations. The population with the larger filling factor has very weak (similar to 150 G) horizontal fields similar to those obtained in previous works. We demonstrate that the field vector of this population is not constrained by the observations, given the spatial resolution and polarimetric accuracy of our data. The topology of the other component with the smaller filling factor is constrained by the observations for field strengths above 250 G: we infer hG fields with inclinations and azimuth values compatible with an isotropic distribution. The filling factors are typically below 30%. We also find that the flux of the two polarities is not balanced. From the other half of the observed quiet-Sun area similar to 50% are two-lobed Stokes V profiles, meaning that 23% of the field of view can be adequately explained with a single constant magnetic field embedded in a non-magnetic atmosphere. The magnetic field vector and filling factor are reliable inferred in only 50% based on the regular profiles. Therefore, 12% of the field of view harbour hG fields with filling factors typically below 30%. At our present spatial resolution, 70% of the pixels apparently are non-magnetised.
In this paper we report on a long multi-wavelength observational campaign of the supergiant fast X-ray transient prototype IGR J17544-2619. A 150 ks-long observation was carried out simultaneously with XMM-Newton and NuSTAR, catching the source in an initial faint X-ray state and then undergoing a bright X-ray outburst lasting approximately 7 ks. We studied the spectral variability during outburst and quiescence by using a thermal and bulk Comptonization model that is typically adopted to describe the X-ray spectral energy distribution of young pulsars in high mass X-ray binaries. Although the statistics of the collected X-ray data were relatively high, we could neither confirm the presence of a cyclotron line in the broad-band spectrum of the source (0.5-40 keV), nor detect any of the previously reported tentative detections of the source spin period. The monitoring carried out with Swift/XRT during the same orbit of the system observed by XMM-Newton and NuSTAR revealed that the source remained in a low emission state for most of the time, in agreement with the known property of all supergiant fast X-ray transients being significantly sub-luminous compared to other supergiant X-ray binaries. Optical and infrared observations were carried out for a total of a few thousand seconds during the quiescence state of the source detected by XMM-Newton and NuSTAR. The measured optical and infrared magnitudes were slightly lower than previous values reported in the literature, but compatible with the known micro-variability of supergiant stars. UV observations obtained with the UVOT telescope on-board Swift did not reveal significant changes in the magnitude of the source in this energy domain compared to previously reported values.
We demonstrate in situ recorded motion of nano-objects adsorbed on a photosensitive polymer film. The motion is induced by a mass transport of the underlying photoresponsive polymer material occurring during irradiation with interference pattern. The polymer film contains azobenzene molecules that undergo reversible photoisomerization reaction from trans-to cis-conformation. Through a multi-scale chain of physico-chemical processes, this finally results in the macro-deformations of the film due to the changing elastic properties of polymer. The topographical deformation of the polymer surface is sensitive to a local distribution of the electrical field vector that allows for the generation of dynamic changes in the surface topography during irradiation with different light interference patterns. Polymer film deformation together with the motion of the adsorbed nano-particles are recorded using a homemade set-up combining an optical part for the generation of interference patterns and an atomic force microscope for acquiring the surface deformation. The particles undergo either translational or rotational motion. The direction of particle motion is towards the topography minima and opposite to the mass transport within the polymer film. The ability to relocate particles by photo-induced dynamic topography fluctuation offers a way for a non-contact simultaneous manipulation of a large number of adsorbed particles just in air at ambient conditions.
Air pollution is the number one environmental cause of premature deaths in Europe. Despite extensive regulations, air pollution remains a challenge, especially in urban areas. For studying summertime air quality in the Berlin–Brandenburg region of Germany, the Weather Research and Forecasting Model with Chemistry (WRF-Chem) is set up and evaluated against meteorological and air quality observations from monitoring stations as well as from a field campaign conducted in 2014. The objective is to assess which resolution and level of detail in the input data is needed for simulating urban background air pollutant concentrations and their spatial distribution in the Berlin–Brandenburg area. The model setup includes three nested domains with horizontal resolutions of 15, 3 and 1 km and anthropogenic emissions from the TNO-MACC III inventory. We use RADM2 chemistry and the MADE/SORGAM aerosol scheme. Three sensitivity simulations are conducted updating input parameters to the single-layer urban canopy model based on structural data for Berlin, specifying land use classes on a sub-grid scale (mosaic option) and downscaling the original emissions to a resolution of ca. 1 km × 1 km for Berlin based on proxy data including traffic density and population density. The results show that the model simulates meteorology well, though urban 2 m temperature and urban wind speeds are biased high and nighttime mixing layer height is biased low in the base run with the settings described above. We show that the simulation of urban meteorology can be improved when specifying the input parameters to the urban model, and to a lesser extent when using the mosaic option. On average, ozone is simulated reasonably well, but maximum daily 8 h mean concentrations are underestimated, which is consistent with the results from previous modelling studies using the RADM2 chemical mechanism. Particulate matter is underestimated, which is partly due to an underestimation of secondary organic aerosols. NOx (NO + NO2) concentrations are simulated reasonably well on average, but nighttime concentrations are overestimated due to the model's underestimation of the mixing layer height, and urban daytime concentrations are underestimated. The daytime underestimation is improved when using downscaled, and thus locally higher emissions, suggesting that part of this bias is due to deficiencies in the emission input data and their resolution. The results further demonstrate that a horizontal resolution of 3 km improves the results and spatial representativeness of the model compared to a horizontal resolution of 15 km. With the input data (land use classes, emissions) at the level of detail of the base run of this study, we find that a horizontal resolution of 1 km does not improve the results compared to a resolution of 3 km. However, our results suggest that a 1 km horizontal model resolution could enable a detailed simulation of local pollution patterns in the Berlin–Brandenburg region if the urban land use classes, together with the respective input parameters to the urban canopy model, are specified with a higher level of detail and if urban emissions of higher spatial resolution are used.
Interplay of coupling and common noise at the transition to synchrony in oscillator populations
(2016)
There are two ways to synchronize oscillators: by coupling and by common forcing, which can be pure noise. By virtue of the Ott-Antonsen ansatz for sine-coupled phase oscillators, we obtain analytically tractable equations for the case where both coupling and common noise are present. While noise always tends to synchronize the phase oscillators, the repulsive coupling can act against synchrony, and we focus on this nontrivial situation. For identical oscillators, the fully synchronous state remains stable for small repulsive coupling; moreover it is an absorbing state which always wins over the asynchronous regime. For oscillators with a distribution of natural frequencies, we report on a counter-intuitive effect of dispersion (instead of usual convergence) of the oscillators frequencies at synchrony; the latter effect disappears if noise vanishes.
The physical properties of galactic winds are one of the keys to understand galaxy formation and evolution. These properties can be constrained thanks to background quasar lines of sight (LOS) passing near star-forming galaxies (SFGs). We present the first results of the MusE GAs FLOw and Wind survey obtained from two quasar fields, which have eight Mg II absorbers of which three have rest equivalent width greater than 0.8 angstrom. With the new Multi Unit Spectroscopic Explorer (MUSE) spectrograph on the Very Large Telescope (VLT), we detect six (75%) Mg II host galaxy candidates within a radius of 30. from the quasar LOS. Out of these six galaxy-quasar pairs, from geometrical argument, one is likely probing galactic outflows, where two are classified as "ambiguous,"two are likely probing extended gaseous disks and one pair seems to be a merger. We focus on the wind-pair and constrain the outflow using a high-resolution quasar spectra from the Ultraviolet and Visual Echelle Spectrograph. Assuming the metal absorption to be due to ga;s flowing out of the detected galaxy through a cone along the minor axis, we find outflow velocities in the order of approximate to 150 km s(-1) (i.e., smaller than the escape velocity) with a loading factor, eta = M-out/SFR, of approximate to 0.7. We see evidence for an open conical flow, with a low-density inner core. In the future, MUSE will provide us with about 80 multiple galaxy-quasar pairs in two dozen fields.
Holographic Structuring of Elastomer Actuator: First True Monolithic Tunable Elastomer Optics
(2016)
Volume diffraction gratings (VDGs) are inscribed selectively by diffusive introduction of benzophenone and subsequent UV-holographic structuring into an electroactive dielectric elastomer actuator (DEA), to afford a continuous voltage-controlled grating shift of 17%. The internal stress coupling of DEA and optical domain allows for a new generation of true monolithic tunable elastomer optics with voltage controlled properties.
We investigate the influence of the Coriolis force on mass motion related to the Rheasilvia impact on asteroid Vesta. Observations by the NASA Dawn mission revealed a pattern of curved radial ridges, which are related to Coriolis-deflected mass-wasting during the initial modification stage of the crater. Utilizing the projected curvature of the mass-wasting trajectories, we developed a method that enabled investigation of the initial mass wasting of the Rheasilvia impact by observational means. We demonstrate that the Coriolis force can strongly affect the crater formation processes on rapidly rotating objects, and we derive the material's velocities (28.9 ± 22.5 m/s), viscosities (1.5–9.0 × 106 Pa s) and coefficients of friction (0.02–0.81) during the impact modification stage. The duration of the impact modification stage could be estimated to (1.1 ± 0.5) h. By analyzing the velocity distribution with respect to the topography, we deduce that the Rheasilvia impactor hit a heterogeneous target and that the initial crater walls were significantly steeper during the modification stage.
Monitoring Ultrafast Chemical Dynamics by Time-Domain X-ray Photo- and Auger-Electron Spectroscopy
(2016)
The directed flow of charge and energy is at the heart of all chemical processes. Extraordinary efforts are underway to monitor and understand the concerted motion of electrons and nuclei with ever increasing spatial and temporal sensitivity. The element specificity, chemical sensitivity, and temporal resolution of ultrafast X-ray spectroscopy techniques hold great promise to provide new insight into the fundamental interactions underlying chemical dynamics in systems ranging from isolated molecules to application-like devices. Here, we focus on the potential of ultrafast X-ray spectroscopy techniques based on the detection of photo- and Auger electrons to provide new fundamental insight into photochemical processes of systems with various degrees of complexity. Isolated nucleobases provide an excellent testing ground for our most fundamental understanding of intramolecular coupling between electrons and nuclei beyond the traditionally applied Born-Oppenheimer approximation. Ultrafast electronic relaxation dynamics enabled by the breakdown of this approximation is the major component of the nucleobase photoprotection mechanisms. Transient X-ray induced Auger electron spectroscopy on photoexcited thymine molecules provides atomic-site specific details of the extremely efficient coupling that converts potentially bond changing ultraviolet photon energy into benign heat. In particular, the time-dependent spectral shift of a specific Auger band is sensitive to the length of a single bond within the molecule. The X-ray induced Auger transients show evidence for an electronic transition out of the initially excited state within only similar to 200 fs in contrast to theoretically predicted picosecond population trapping behind a reaction barrier. Photoinduced charge transfer dynamics between transition metal complexes and semiconductor nanostructures are of central importance for many emerging energy and climate relevant technologies. Numerous demonstrations of photovoltaic and photocatalytic activity have been performed based on the combination of strong light absorption in dye molecules with charge separation and transport in adjacent semiconductor nanostructures. However, a fundamental understanding of the enabling and limiting dynamics on critical atomic length- and time scales is often still lacking. Femtosecond time-resolved X-ray photoelectron spectroscopy is employed to gain a better understanding of a short-lived intermediate that may be linked to the unexpectedly limited performance of ZnO based dye-sensitized solar cells by delaying the generation of free charge carriers. The transient spectra strongly suggest that photoexcited dye molecules attached to ZnO nanocrystals inject their charges into the substrate within less than 1 ps but the electrons are then temporarily trapped at the surface of the semiconductor in direct vicinity of the injecting molecules. The experiments are extended to monitor the electronic response of the semiconductor substrate to the collective injection from a monolayer of dye molecules and the subsequent electron-ion recombination dynamics. The results indicate some qualitative similarities but quantitative differences between the recombination dynamics at molecule-semiconductor interfaces and previously studied bulk-surface electron-hole recombination dynamics in photoexcited semiconductors.
In a network with a mixture of different electrophysiological types of neurons linked by excitatory and inhibitory connections, temporal evolution leads through repeated epochs of intensive global activity separated by intervals with low activity level. This behavior mimics "up" and "down" states, experimentally observed in cortical tissues in absence of external stimuli. We interpret global dynamical features in terms of individual dynamics of the neurons. In particular, we observe that the crucial role both in interruption and in resumption of global activity is played by distributions of the membrane recovery variable within the network. We also demonstrate that the behavior of neurons is more influenced by their presynaptic environment in the network than by their formal types, assigned in accordance with their response to constant current.
In the study of relativistic jets one of the key open questions is their interaction with the environment on the microscopic level. Here, we study the initial evolution of both electron-proton (e(-)-p(+)) and electron-positron (e(+/-)) relativistic jets containing helical magnetic fields, focusing on their interaction with an ambient plasma. We have performed simulations of "global" jets containing helical magnetic fields in order to examine how helical magnetic fields affect kinetic instabilities such as the Weibel instability, the kinetic Kelvin-Helmholtz instability (kKHI) and the Mushroom instability (MI). In our initial simulation study these kinetic instabilities are suppressed and new types of instabilities can grow. In the e(-)-p(+) jet simulation a recollimation-like instability occurs and jet electrons are strongly perturbed. In the e(+/-) jet simulation a recollimation-like instability occurs at early times followed by a kinetic instability and the general structure is similar to a simulation without helical magnetic field. Simulations using much larger systems are required in order to thoroughly follow the evolution of global jets containing helical magnetic fields.
We do magnetohydrodynamic (MHD) simulations of local box models of turbulent Interstellar Medium (ISM) and analyse the process of amplification and saturation of mean magnetic fields with methods of mean field dynamo theory. It is shown that the process of saturation of mean fields can be partially described by the prolonged diffusion time scales in presence of the dynamically significant magnetic fields. However, the outward wind also plays an essential role in the saturation in higher SN rate case. Algebraic expressions for the back reaction of the magnetic field onto the turbulent transport coefficients are derived, which allow a complete description of the nonlinear dynamo. We also present the effects of dynamically significant mean fields on the ISM configuration and pressure distribution. We further add the cosmic ray component in the simulations and investigate the kinematic growth of mean fields with a dynamo perspective.
The Milky Way is only one out of billions of galaxies in the universe. However, it is a special galaxy because it allows to explore the main mechanisms involved in its evolution and formation history by unpicking the system star-by-star. Especially, the chemical fingerprints of its stars provide clues and evidence of past events in the Galaxy’s lifetime. These information help not only to decipher the current structure and building blocks of the Milky Way, but to learn more about the general formation process of galaxies.
In the past decade a multitude of stellar spectroscopic Galactic surveys have scanned millions of stars far beyond the rim of the solar neighbourhood. The obtained spectroscopic information provide unprecedented insights to the chemo-dynamics of the Milky Way. In addition analytic models and numerical simulations of the Milky Way provide necessary descriptions and predictions suited for comparison with observations in order to decode the physical properties that underlie the complex system of the Galaxy.
In the thesis various approaches are taken to connect modern theoretical modelling of galaxy formation and evolution with observations from Galactic stellar surveys. With its focus on the chemo-kinematics of the Galactic disk this work aims to determine new observational constraints on the formation of the Milky Way providing also proper comparisons with two different models. These are the population synthesis model TRILEGAL based on analytical distribution functions, which aims to simulate the number and distribution of stars in the Milky Way and its different components, and a hybrid model (MCM) that combines an N-body simulation of a Milky Way like galaxy in the cosmological framework with a semi-analytic chemical evolution model for the Milky Way. The major observational data sets in use come from two surveys, namely the “Radial Velocity Experiment” (RAVE) and the “Sloan Extension for Galactic Understanding and Exploration” (SEGUE).
In the first approach the chemo-kinematic properties of the thin and thick disk of the Galaxy as traced by a selection of about 20000 SEGUE G-dwarf stars are directly compared to the predictions by the MCM model. As a necessary condition for this, SEGUE's selection function and its survey volume are evaluated in detail to correct the spectroscopic observations for their survey specific selection biases. Also, based on a Bayesian method spectro-photometric distances with uncertainties below 15% are computed for the selection of SEGUE G-dwarfs that are studied up to a distance of 3 kpc from the Sun.
For the second approach two synthetic versions of the SEGUE survey are generated based on the above models. The obtained synthetic stellar catalogues are then used to create mock samples best resembling the compiled sample of observed SEGUE G-dwarfs. Generally, mock samples are not only ideal to compare predictions from various models. They also allow validation of the models' quality and improvement as with this work could be especially achieved for TRILEGAL. While TRILEGAL reproduces the statistical properties of the thin and thick disk as seen in the observations, the MCM model has shown to be more suitable in reproducing many chemo-kinematic correlations as revealed by the SEGUE stars. However, evidence has been found that the MCM model may be missing a stellar component with the properties of the thick disk that the observations clearly show. While the SEGUE stars do indicate a thin-thick dichotomy of the stellar Galactic disk in agreement with other spectroscopic stellar studies, no sign for a distinct metal-poor disk is seen in the MCM model.
Usually stellar spectroscopic surveys are limited to a certain volume around the Sun covering different regions of the Galaxy’s disk. This often prevents to obtain a global view on the chemo-dynamics of the Galactic disk. Hence, a suitable combination of stellar samples from independent surveys is not only useful for the verification of results but it also helps to complete the picture of the Milky Way. Therefore, the thesis closes with a comparison of the SEGUE G-dwarfs and a sample of RAVE giants. The comparison reveals that the chemo-kinematic relations agree in disk regions where the samples of both surveys show a similar number of stars. For those parts of the survey volumes where one of the surveys lacks statistics they beautifully complement each other. This demonstrates that the comparison of theoretical models on the one side, and the combined observational data gathered by multiple surveys on the other side, are key ingredients to understand and disentangle the structure and formation history of the Milky Way.
In the current paradigm of cosmology, the formation of large-scale structures is mainly driven by non-radiating dark matter, making up the dominant part of the matter budget of the Universe. Cosmological observations however, rely on the detection of luminous galaxies, which are biased tracers of the underlying dark matter. In this thesis I present cosmological reconstructions of both, the dark matter density field that forms the cosmic web, and cosmic velocities, for which both aspects of my work are delved into, the theoretical formalism and the results of its applications to cosmological simulations and also to a galaxy redshift survey.The foundation of our method is relying on a statistical approach, in which a given galaxy catalogue is interpreted as a biased realization of the underlying dark matter density field. The inference is computationally performed on a mesh grid by sampling from a probability density function, which describes the joint posterior distribution of matter density and the three dimensional velocity field. The statistical background of our method is described in Chapter ”Implementation of argo”, where the introduction in sampling methods is given, paying special attention to Markov Chain Monte-Carlo techniques. In Chapter ”Phase-Space Reconstructions with N-body Simulations”, I introduce and implement a novel biasing scheme to relate the galaxy number density to the underlying dark matter, which I decompose into a deterministic part, described by a non-linear and scale-dependent analytic expression, and a stochastic part, by presenting a negative binomial (NB) likelihood function that models deviations from Poissonity. Both bias components had already been studied theoretically, but were so far never tested in a reconstruction algorithm. I test these new contributions againstN-body simulations to quantify improvements and show that, compared to state-of-the-art methods, the stochastic bias is inevitable at wave numbers of k≥0.15h Mpc^−1 in the power spectrum in order to obtain unbiased results from the reconstructions. In the second part of Chapter ”Phase-Space Reconstructions with N-body Simulations” I describe and validate our approach to infer the three dimensional cosmic velocity field jointly with the dark matter density. I use linear perturbation theory for the large-scale bulk flows and a dispersion term to model virialized galaxy motions, showing that our method is accurately recovering the real-space positions of the redshift-space distorted galaxies. I analyze the results with the isotropic and also the two-dimensional power spectrum.Finally, in Chapter ”Phase-space Reconstructions with Galaxy Redshift Surveys”, I show how I combine all findings and results and apply the method to the CMASS (for Constant (stellar) Mass) galaxy catalogue of the Baryon Oscillation Spectroscopic Survey (BOSS). I describe how our method is accounting for the observational selection effects inside our reconstruction algorithm. Also, I demonstrate that the renormalization of the prior distribution function is mandatory to account for higher order contributions in the structure formation model, and finally a redshift-dependent bias factor is theoretically motivated and implemented into our method. The various refinements yield unbiased results of the dark matter until scales of k≤0.2 h Mpc^−1in the power spectrum and isotropize the galaxy catalogue down to distances of r∼20h^−1 Mpc in the correlation function. We further test the results of our cosmic velocity field reconstruction by comparing them to a synthetic mock galaxy catalogue, finding a strong correlation between the mock and the reconstructed velocities. The applications of both, the density field without redshift-space distortions, and the velocity reconstructions, are very broad and can be used for improved analyses of the baryonic acoustic oscillations, environmental studies of the cosmic web, the kinematic Sunyaev-Zel’dovic or integrated Sachs-Wolfe effect.
In der vorliegenden Arbeit wird die planetare Grenzschicht in Ny-Ålesund, Spitzbergen, sowohl bezüglich kleinskaliger („mikrometeorologischer“) Effekte als auch in ihrer Kopplung mit der Synoptik untersucht. Dazu werden verschiedene Beobachtungsdaten aus der Säule und in Bodennähe zusammengezogen und bewertet. Die so gewonnenen Datensätze werden dann zur Validierung eines nicht-hydrostatischen, regionalen Klimamodells genutzt. Weiterhin werden orographisch bedingte Einflüsse, die Untergrundbeschaffenheit und die lokale Heterogenität der Unterlage untersucht. Hierzu werden meteorologische Größen, wie die Variabilität der Temperatur und insbesondere die jährliche Windverteilung in Bodennähe untersucht und es erfolgt ein Vergleich von in-situ gemessenen turbulenten Flüssen von den Eddy-Kovarianz-Messkomplexen bei Ny-Ålesund und im Bayelva-Tal unter demselben Aspekt. Es zeigt sich, dass der Eddy-Kovarianz-Messkomplex im Bayelva-Tal sehr stark durch eine orographisch bedingte Kanalisierung der Strömung beeinflusst ist und sich nicht für Vergleiche mit regionalen Klimamodellen mit horizontalen Auflösungen von <1km eignet. Die hohe Bodenfeuchte im Bayelva-Tal führt zudem zu einem deutlich kleineren Bowen-Verhältnis, als es für diese Region zu erwarten ist. Der Eddy-Kovarianz-Messkomplex bei Ny-Ålesund erweist sich hingegen als geeigneter für solche Modellvergleiche, aufgrund der typischen, küstennahen Windverteilung und des repräsentativen Footprints. Letzteres wird durch die Bestimmung der Footprint-Klimatologie des Jahres 2013 mit einem aktuellen Footprint-Modell erarbeitet.
Weiterhin wird die Auswirkung von (Anti-) Zyklonen über den Archipel auf die zeitliche Variabilität der lokalen Grenzschichteigenschaften untersucht und bewertet. Dazu wird ein Zyklonen-Detektions-Algorithmus auf ERA-Interim-Reanalysedatensätze angewendet, wodurch die Häufigkeit von nahezu ideal konzentrischen Hoch- und die Tiefdruckgebieten für drei Jahre bestimmt wird. Aus dieser Verteilung werden insgesamt drei interessante Zeiträume zu verschiedenen Jahreszeiten ausgewählt und im Rahmen von Prozessstudien die lokalen bodennahen meteorologischen Messungen, der turbulente Austausch an der Oberfläche und die Grenzschichtdynamik in der Säule untersucht. Die zeitliche Variabilität der dynamischen Grenzschichtstabilität in der Säule wird anhand von zeitlich hoch aufgelösten vertikalen Profilen der Bulk-Richardson-Zahl aus Kompositprofilen aus Fernerkundungsinstrumenten (Radiometer, Wind-LIDAR) sowie Mastdaten (BSRN-Mast) untersucht und die Grenzschichthöhe ermittelt. Aus diesen Analysen ergibt sich eine deutliche Abhängigkeit der thermischen Stabilität beim Durchzug von Fronten, eine damit einhergehende erhebliche Abhängigkeit der Grenzschichtdynamik und der Grenzschichthöhe sowie des turbulenten Austauschs von der zeitlichen Variabilität der Windgeschwindigkeit in der Säule.
Auf Grundlage der Standortanalysen und Prozessstudien erfolgt ein Vergleich der bodennahen Messungen und den Beobachtungen aus der Säule, sowohl von den genannten Fernerkundungsinstrumenten als auch von In-situ-Messungen (Radiosonden) für den Zeitraum einer Radiosondierungskampagne mit dem nicht-hydrostatischen, regionalen Klimamodel WRF (ARW). Auf Grundlage der Fragestellung, inwieweit aktuelle Schemata die Grenzschichtcharakteristika in orographisch stark gegliedertem Gelände in der Arktis reproduzieren können, werden zwei Grenzschichtparametrisierungsschemata mit verschiedenen Ordnungen der Schließung validiert. Hierzu wird die zeitliche Variabilität der Temperatur, der Feuchte und des Windfeldes in der Säule bis 2000m in den Simulationen mit den Beobachtungsdaten vergleichen. Es wird gezeigt, dass durch Modifikation der Initialwertfelder eine sehr gute Übereinstimmung zwischen den Simulationen und den Beobachtungen bereits bei einer horizontalen Auflösung von 1km erreicht werden kann und die Wahl des Grenzschichtschemas nur untergeordneten Einfluss hat. Hieraus werden Ansätze der Weiterentwicklung der Parametrisierungen, aber auch Empfehlungen bezüglich der Initialwertfelder, wie der Landmaske und der Orographie, vorgeschlagen.
This work reports about new high-resolution imaging and spectroscopic observations of solar type III radio bursts at low radio frequencies in the range from 30 to 80 MHz. Solar type III radio bursts are understood as result of the beam-plasma interaction of electron beams in the corona. The Sun provides a unique opportunity to study these plasma processes of an active star. Its activity appears in eruptive events like flares, coronal mass ejections and radio bursts which are all accompanied by enhanced radio emission. Therefore solar radio emission carries important information about plasma processes associated with the Sun’s activity. Moreover, the Sun’s atmosphere is a unique plasma laboratory with plasma processes under conditions not found in terrestrial laboratories. Because of the Sun’s proximity to Earth, it can be studied in greater detail than any other star but new knowledge about the Sun can be transfer to them. This “solar stellar connection” is important for the understanding of processes on other stars.
The novel radio interferometer LOFAR provides imaging and spectroscopic capabilities to study these processes at low frequencies. Here it was used for solar observations.
LOFAR, the characteristics of its solar data and the processing and analysis of the latter with the Solar Imaging Pipeline and Solar Data Center are described. The Solar Imaging Pipeline is the central software that allows using LOFAR for solar observations. So its development was necessary for the analysis of solar LOFAR data and realized here. Moreover a new density model with heat conduction and Alfvén waves was developed that provides the distance of radio bursts to the Sun from dynamic radio spectra.
Its application to the dynamic spectrum of a type III burst observed on March 16, 2016 by LOFAR shows a nonuniform radial propagation velocity of the radio emission. The analysis of an imaging observation of type III bursts on June 23, 2012 resolves a burst as bright, compact region localized in the corona propagating in radial direction along magnetic field lines with an average velocity of 0.23c. A nonuniform propagation velocity is revealed. A new beam model is presented that explains the nonuniform motion of the radio source as a propagation effect of an electron ensemble with a spread velocity distribution and rules out a monoenergetic electron distribution. The coronal electron number density is derived in the region from 1.5 to 2.5 R☉ and fitted with the newly developed density model. It determines the plasma density for the interplanetary space between Sun and Earth. The values correspond to a 1.25- and 5-fold Newkirk model for harmonic and fundamental emission, respectively. In comparison to data from other radio instruments the LOFAR data shows a high sensitivity and resolution in space, time and frequency.
The new results from LOFAR’s high resolution imaging spectroscopy are consistent with current theories of solar type III radio bursts and demonstrate its capability to track fast moving radio sources in the corona. LOFAR solar data is found to be a valuable source for solar radio physics and opens a new window for studying plasma processes associated with highly energetic electrons in the solar corona.
Solar-like stars maintain their magnetic fields thanks to a dynamo mechanism. The Babcock-Leighton dynamo is one possible dynamo that has the particularity to require magnetic flux tubes. Magnetic flux tubes are assumed to form at the bottom of the convective zone and rise buoyantly to the surface. A delayed dynamo model has been suggested, where the delay accounts for the rise time of the magnetic flux tubes; a time, that has been ignored by former studies.
The present thesis aims to study the applicability of the flux tube/Babcock-Leighton dynamo to other stars. To do so, we attempt to constrain the rise time of magnetic flux tubes thanks to the first fully compressible MHD simulations of rising magnetic flux tubes in stratified rotating spherical shells.
Such simulations are limited to an unrealistic parameter space, therefore, a scaling relation is required to scale the results to realistic physical regimes. We extended earlier works on 2D scaling relations and derived a general scaling law valid for both 2D and 3D. We then carried out two large series of numerical experiments and verified that the scaling law we have derived indeed applies to the fully non-linear case. It allowed us to extract a constraint for the rise time of magnetic flux tubes that is valid for any solar-like star. We finally introduced this constraint to a delayed dynamo model.
By carrying out simulations of a mean-field, delayed, flux tube/Babcock-Leighton dynamo, we were able to identify a new dynamo regime resulting from the delay. This regime requires delays about an entire cycle and exhibits subequipartition magnetic activity. Revealing this new regime shows that even for long delays the flux tube/Babcock-Leighton dynamo can still deliver non-decaying solutions and remains a good candidate for a wide range of solar-like stars.
In this paper we report an experimental and computational study of liquid acetonitrile (H3C–C[triple bond, length as m-dash]N) by resonant inelastic X-ray scattering (RIXS) at the N K-edge. The experimental spectra exhibit clear signatures of the electronic structure of the valence states at the N site and incident-beam-polarization dependence is observed as well. Moreover, we find fine structure in the quasielastic line that is assigned to finite scattering duration and nuclear relaxation. We present a simple and light-to-evaluate model for the RIXS maps and analyze the experimental data using this model combined with ab initio molecular dynamics simulations. In addition to polarization-dependence and scattering-duration effects, we pinpoint the effects of different types of chemical bonding to the RIXS spectrum and conclude that the H2C–C[double bond, length as m-dash]NH isomer, suggested in the literature, does not exist in detectable quantities. We study solution effects on the scattering spectra with simulations in liquid and in vacuum. The presented model for RIXS proved to be light enough to allow phase-space-sampling and still accurate enough for identification of transition lines in physical chemistry research by RIXS.
We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution.
In the first part of my work I have investigated the ageing properties of the first passage time distributions in a one-dimensional subdiffusive continuous time random walk with power law distributed waiting times of the form $\psi(\tau) \sim \tau^{-1-\alpha}$ with $0<\alpha<1$ and $1<\alpha<2$. The age or ageing time $t_a$ is the time span from the start of the stochastic process to the start of the observation of this process (at $t=0$). I have calculated the results for a single target and two targets, also including the biased case, where the walker is driven towards the boundary by a constant force. I have furthermore refined the previously derived results for the non-ageing case and investigated the changes that occur when the walk is performed in a discrete quenched energy landscape, where the waiting times are fixed for every site. The results include the exact Laplace space densities and infinite (converging) series as exact results in the time space. The main results are the dominating long time power law behavior regimes, which depend on the ageing time. For the case of unbiased subdiffusion ($\alpha < 1$) in the presence of one target, I find three different dominant terms for ranges of $t$ separated by $t_a$ and another crossover time $t^{\star}$, which depends on $t_a$ as well as on the anomalous exponent $\alpha$ and the anomalous diffusion coefficient $K_{\alpha}$. In all three regimes ($t \ll t_a$, $t_a \ll t \ll t^{\star}$, $t \gg t^{\star}$) one finds power law decay with exponents depending on $\alpha$. The middle regime only exists for $t_a \ll t^{\star}$. The dominant terms in the first two regimes (ageing regimes) come from the probability distribution of the forward waiting time, the time one has to wait for the stochastic process to make the first step during the observation. When the observation time is larger than the second crossover time $t^{\star}$, the first passage time density does not show ageing and the non-ageing first passage time dominates. The power law exponents in the respective regimes are $-\alpha$ for strong ageing, $-1-\alpha$ in the intermediate regime, and $-1-\alpha/2$ in the final non-ageing regime. A similar split into three regimes can be found for $1<\alpha<2$, only with a different second crossover time $t^*$. In this regime the diffusion is normal but also age-dependent. For the diffusion in quenched energy landscapes one cannot detect ageing. The first passage time density shows a quenched power law $^\sim t^{-(1+2\alpha)/(1+\alpha)}$. For diffusion between two target sites and the biased diffusion towards a target only two scaling regimes emerge, separated by the ageing time. In the ageing case $t \ll t_a$ the forward waiting time is again dominant with power law exponent $-\alpha$, while the non-ageing power law $-1-\alpha$ is found for all times $t \gg t_a$. An intermediate regime does not exist. The bias and the confinement have similar effects on the first passage time density. For quenched diffusion, the biased case is interesting, as the bias reduces correlations due to revisiting of the same waiting time. As a result, CTRW like behavior is observed, including ageing. Extensive computer simulations support my findings.
The second part of my research was done on the subject of ageing Scher-Montroll transport, which is in parts closely related to the first passage densities. It explains the electrical current in an amorphous material. I have investigated the effect of the width of a given initial distribution of charge carriers on the transport coefficients as well as the ageing effect on the emerging power law regimes and a constant initial regime. While a spread out initial distribution has only little impact on the Scher-Montroll current, ageing alters the behavior drastically. Instead of the two classical power laws one finds four current regimes, up to three of which can appear in a single experiment. The dominant power laws differ for $t \ll t_a, t_c$, $t_a \ll t \ll t_c$, $t_c \ll t \ll t_a$, and $t \gg t_a,t_c$. Here, $t_c$ is the crossover time of the non-aged Scher-Montroll current. For strongly aged systems one can observe a constant current in the first regime while the others are dominated by decaying power laws with exponents $\alpha -1$, $-\alpha$, and $-1-\alpha$. The ageing regimes are the 1st and 3rd one, while the classical regimes are the 2nd and the 4th. I have verified the theory using numerical integration of the exact integrals and applied the new results to experimental data.
In the third part I considered a single file of subdiffusing particles in an energy landscape. Every occupied site of the landscape acts as a boundary, from which a particle is immediately reflected to its previous site, if it tries to jump there. I have analysed the effects single-file diffusion a quenched landscape compared to an annealed landscape and I have related these results to the number of steps and related quantities. The diffusion changes from ultraslow logarithmic diffusion in the annealed or CTRW case to subdiffusion with an anomalous exponent $\alpha/(1+\alpha)$ in the quenched landscape. The behavior is caused by the forward waiting time, which changes drastically from the quenched to the annealed case. Single-file effects in the quenched landscape are even more complicated to consider in the ensemble average, since the diffusion in individual landscapes shows extremely diverse behavior. Extensive simulations support my theoretical arguments, which consider mainly the long time evolution of the mean square displacement of a bulk particle.
Interplay of coupling and common noise at the transition to synchrony in oscillator populations
(2016)
There are two ways to synchronize oscillators: by coupling and by common forcing, which can be pure noise. By virtue of the Ott-Antonsen ansatz for sine-coupled phase oscillators, we obtain analytically tractable equations for the case where both coupling and common noise are present. While noise always tends to synchronize the phase oscillators, the repulsive coupling can act against synchrony, and we focus on this nontrivial situation. For identical oscillators, the fully synchronous state remains stable for small repulsive coupling; moreover it is an absorbing state which always wins over the asynchronous regime. For oscillators with a distribution of natural frequencies, we report on a counter-intuitive effect of dispersion (instead of usual convergence) of the oscillators frequencies at synchrony; the latter effect disappears if noise vanishes.
In this thesis we use integral-field spectroscopy to detect and understand of Lyman α (Lyα) emission from high-redshift galaxies.
Intrinsically the Lyα emission at λ = 1216 Å is the strongest recombination line from galaxies. It arises from the 2p → 1s transition in hydrogen. In star-forming galaxies the line is powered by ionisation of the interstellar gas by hot O- and B- stars. Galaxies with star-formation rates of 1 - 10 Msol/year are expected to have Lyα luminosities of 42 dex - 43 dex (erg/s), corresponding to fluxes ~ -17 dex - -18 dex (erg/s/cm²) at redshifts z~3, where Lyα is easily accessible with ground-based telescopes. However, star-forming galaxies do not show these expected Lyα fluxes. Primarily this is a consequence of the high-absorption cross-section of neutral hydrogen for Lyα photons σ ~ -14 dex (cm²). Therefore, in typical interstellar environments Lyα photons have to undergo a complex radiative transfer. The exact conditions under which Lyα photons can escape a galaxy are poorly understood.
Here we present results from three observational projects. In Chapter 2, we show integral field spectroscopic observations of 14 nearby star-forming galaxies in Balmer α radiation (Hα, λ = 6562.8 Å). These observations were obtained with the Potsdam Multi Aperture Spectrophotometer at the Calar-Alto 3.5m Telescope}. Hα directly traces the intrinsic Lyα radiation field. We present Hα velocity fields and velocity dispersion maps spatially registered onto Hubble Space Telescope Lyα and Hα images. From our observations, we conjecture a causal connection between spatially resolved Hα kinematics and Lyα photometry for individual galaxies. Statistically, we find that dispersion-dominated galaxies are more likely to emit Lyα photons than galaxies where ordered gas-motions dominate. This result indicates that turbulence in actively star-forming systems favours an escape of Lyα radiation.
Not only massive stars can power Lyα radiation, but also non-thermal emission from an accreting super-massive black hole in the galaxy centre. If a galaxy harbours such an active galactic nucleus, the rate of hydrogen-ionising photons can be more than 1000 times higher than that of a typical star-forming galaxy. This radiation can potentially ionise large regions well outside the main stellar body of galaxies. Therefore, it is expected that the neutral hydrogen from these circum-galactic regions shines fluorescently in Lyα. Circum-galactic gas plays a crucial role in galaxy formation. It may act as a reservoir for fuelling star formation, and it is also subject to feedback processes that expel galactic material. If Lyα emission from this circum-galactic medium (CGM) was detected, these important processes could be studied in-situ around high-z galaxies. In Chapter 3, we show observations of five radio-quiet quasars with PMAS to search for possible extended CGM emission in the Lyα line. However, in four of the five objects, we find no significant traces of this emission. In the fifth object, there is evidence for a weak and spatially quite compact Lyα excess at several kpc outside the nucleus. The faintness of these structures is consistent with the idea that radio-quiet quasars typically reside in dark matter haloes of modest masses. While we were not able to detect Lyα CGM emission, our upper limits provide constraints for the new generation of IFS instruments at 8--10m class telescopes.
The Multi Unit Spectroscopic Explorer (MUSE) at ESOs Very Large Telescopeis such an unique instrument. One of the main motivating drivers in its construction was the use as a survey instrument for Lyα emitting galaxies at high-z. Currently, we are conducting such a survey that will cover a total area of ~100 square arcminutes with 1 hour exposures for each 1 square arcminute MUSE pointing. As a first result from this survey we present in Chapter 5 a catalogue of 831 emission-line selected galaxies from a 22.2 square arcminute region in the Chandra Deep Field South. In order to construct the catalogue, we developed and implemented a novel source detection algorithm -- LSDCat -- based on matched filtering for line emission in 3D spectroscopic datasets (Chapter 4). Our catalogue contains 237 Lyα emitting galaxies in the redshift range 3 ≲ z ≲ 6. Only four of those previously had spectroscopic redshifts in the literature. We conclude this thesis with an outlook on the construction of a Lyα luminosity function based on this unique sample (Chapter 6).
Can the statistical properties of single-electron transfer events be correctly predicted within a common equilibrium ensemble description? This fundamental in nanoworld question of ergodic behavior is scrutinized within a very basic semi-classical curve-crossing problem. It is shown that in the limit of non-adiabatic electron transfer (weak tunneling) well-described by the Marcus–Levich–Dogonadze(MLD) rate the answer is yes. However, in the limit of the so-called solvent-controlled adiabatic electron transfer, a profound breaking of ergodicity occurs. Namely, a common description based on the ensemble reduced density matrix with an initial equilibrium distribution of the reaction coordinate is not able to reproduce the statistics of single-trajectory events in this seemingly classical regime. For sufficiently large activation barriers, the ensemble survival probability in a state remains nearly exponential with the inverse rate given by the sum of the adiabatic curve crossing (Kramers) time and the inverse MLD rate. In contrast, near to the adiabatic regime, the single-electron survival probability is clearly non-exponential, even though it possesses an exponential tail which agrees well with the ensemble description. Initially, it is well described by a Mittag-Leffler distribution with a fractional rate. Paradoxically, the mean transfer time in this classical on the ensemble level regime is well described by the inverse of the nonadiabatic quantum tunneling rate on a single particle level. An analytical theory is developed which perfectly agrees with stochastic simulations and explains our findings.
We introduce azobenzene-functionalized polyelectrolyte multilayers as efficient, inexpensive optoacoustic transducers for hyper-sound strain waves in the GHz range. By picosecond transient reflectivity measurements we study the creation of nanoscale strain waves, their reflection from interfaces, damping by scattering from nanoparticles and propagation in soft and hard adjacent materials like polymer layers, quartz and mica. The amplitude of the generated strain ε ∼ 5 × 10−4 is calibrated by ultrafast X-ray diffraction.
The goal of the presented work is to explore the interaction between gold nanorods (GNRs) and hyper-sound waves. For the generation of the hyper-sound I have used Azobenzene-containing polymer transducers. Multilayer polymer structures with well-defined thicknesses and smooth interfaces were built via layer-by-layer deposition. Anionic polyelectrolytes with Azobenzene side groups (PAzo) were alternated with cationic polymer PAH, for the creation of transducer films. PSS/PAH multilayer were built for spacer layers, which do not absorb in the visible light range. The properties of the PAzo/PAH film as a transducer are carefully characterized by static and transient optical spectroscopy. The optical and mechanical properties of the transducer are studied on the picosecond time scale. In particular the relative change of the refractive index of the photo-excited and expanded PAH/PAzo is Δn/n = - 2.6*10‐4. Calibration of the generated strain is performed by ultrafast X-ray diffraction calibrated the strain in a Mica substrate, into which the hyper-sound is transduced. By simulating the X-ray data with a linear-chain-model the strain in the transducer under the excitation is derived to be Δd/d ~ 5*10‐4.
Additional to the investigation of the properties of the transducer itself, I have performed a series of experiments to study the penetration of the generated strain into various adjacent materials. By depositing the PAzo/PAH film onto a PAH/PSS structure with gold nanorods incorporated in it, I have shown that nanoscale impurities can be detected via the scattering of hyper-sound.
Prior to the investigation of complex structures containing GNRs and the transducer, I have performed several sets of experiments on GNRs deposited on a small buffer of PSS/PAH. The static and transient response of GNRs is investigated for different fluence of the pump beam and for different dielectric environments (GNRs covered by PSS/PAH).
A systematic analysis of sample architectures is performed in order to construct a sample with the desired effect of GNRs responding to the hyper-sound strain wave. The observed shift of a feature related to the longitudinal plasmon resonance in the transient reflection spectra is interpreted as the event of GNRs sensing the strain wave. We argue that the shift of the longitudinal plasmon resonance is caused by the viscoelastic deformation of the polymer around the nanoparticle. The deformation is induced by the out of plane difference in strain in the area directly under a particle and next to it. Simulations based on the linear chain model support this assumption. Experimentally this assumption is proven by investigating the same structure, with GNRs embedded in a PSS/PAH polymer layer.
The response of GNRs to the hyper-sound wave is also observed for the sample structure with GNRs embedded in PAzo/PAH films. The response of GNRs in this case is explained to be driven by the change of the refractive index of PAzo during the strain propagation.
The strong adhesion of sub-micron sized particles to surfaces is a nuisance, both for removing contaminating colloids from surfaces and for conscious manipulation of particles to create and test novel micro/nano-scale assemblies. The obvious idea of using detergents to ease these processes suffers from a lack of control: the action of any conventional surface-modifying agent is immediate and global. With photosensitive azobenzene containing surfactants we overcome these limitations. Such photo-soaps contain optical switches (azobenzene molecules), which upon illumination with light of appropriate wavelength undergo reversible trans-cis photo-isomerization resulting in a subsequent change of the physico-chemical molecular properties. In this work we show that when a spatial gradient in the composition of trans- and cis- isomers is created near a solid-liquid interface, a substantial hydrodynamic flow can be initiated, the spatial extent of which can be set, e.g., by the shape of a laser spot. We propose the concept of light induced diffusioosmosis driving the flow, which can remove, gather or pattern a particle assembly at a solid-liquid interface. In other words, in addition to providing a soap we implement selectivity: particles are mobilized and moved at the time of illumination, and only across the illuminated area.
The strong adhesion of sub-micron sized particles to surfaces is a nuisance, both for removing contaminating colloids from surfaces and for conscious manipulation of particles to create and test novel micro/nano-scale assemblies. The obvious idea of using detergents to ease these processes suffers from a lack of control: the action of any conventional surface-modifying agent is immediate and global. With photosensitive azobenzene containing surfactants we overcome these limitations. Such photo-soaps contain optical switches (azobenzene molecules), which upon illumination with light of appropriate wavelength undergo reversible trans-cis photo-isomerization resulting in a subsequent change of the physico-chemical molecular properties. In this work we show that when a spatial gradient in the composition of trans- and cis- isomers is created near a solid-liquid interface, a substantial hydrodynamic flow can be initiated, the spatial extent of which can be set, e.g., by the shape of a laser spot. We propose the concept of light induced diffusioosmosis driving the flow, which can remove, gather or pattern a particle assembly at a solid-liquid interface. In other words, in addition to providing a soap we implement selectivity: particles are mobilized and moved at the time of illumination, and only across the illuminated area.
We study the adsorption–desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition—demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces—are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye–Hückel approximation is often not feasible and the nonlinear Poisson–Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson–Boltzmann equation is smaller than the Debye–Hückel result, such that the required critical surface charge density for polyelectrolyte adsorption σc increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical–chemical and biophysical systems.
We study the adsorption–desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition—demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces—are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye–Hückel approximation is often not feasible and the nonlinear Poisson–Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson–Boltzmann equation is smaller than the Debye–Hückel result, such that the required critical surface charge density for polyelectrolyte adsorption σc increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical–chemical and biophysical systems.
Thermophony in real gases
(2016)
A thermophone is an electrical device for sound generation. The advantages of thermophones over conventional sound transducers such as electromagnetic, electrostatic or piezoelectric transducers are their operational principle which does not require any moving parts, their resonance-free behavior, their simple construction and their low production costs.
In this PhD thesis, a novel theoretical model of thermophonic sound generation in real gases has been developed. The model is experimentally validated in a frequency range from 2 kHz to 1 MHz by testing more then fifty thermophones of different materials, including Carbon nano-wires, Titanium, Indium-Tin-Oxide, different sizes and shapes for sound generation in gases such as air, argon, helium, oxygen, nitrogen and sulfur hexafluoride.
Unlike previous approaches, the presented model can be applied to different kinds of thermophones and various gases, taking into account the thermodynamic properties of thermophone materials and of adjacent gases, degrees of freedom and the volume occupied by the gas atoms and molecules, as well as sound attenuation effects, the shape and size of the thermophone surface and the reduction of the generated acoustic power due to photonic emission. As a result, the model features better prediction accuracy than the existing models by a factor up to 100. Moreover, the new model explains previous experimental findings on thermophones which can not be explained with the existing models.
The acoustic properties of the thermophones have been tested in several gases using unique, highly precise experimental setups comprising a Laser-Doppler-Vibrometer combined with a thin polyethylene film which acts as a broadband and resonance-free sound-pressure detector. Several outstanding properties of the thermophones have been demonstrated for the first time, including the ability to generate arbitrarily shaped acoustic signals, a greater acoustic efficiency compared to conventional piezoelectric and electrostatic airborne ultrasound transducers, and applicability as powerful and tunable sound sources with a bandwidth up to the megahertz range and beyond.
Additionally, new applications of thermophones such as the study of physical properties of gases, the thermo-acoustic gas spectroscopy, broad-band characterization of transfer functions of sound and ultrasound detection systems, and applications in non-destructive materials testing are discussed and experimentally demonstrated.
We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the Néel temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost.
We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the Néel temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost.
The molecular ability to selectively and efficiently convert sunlight into other forms of energy like heat, bond change, or charge separation is truly remarkable. The decisive steps in these transformations often happen on a femtosecond timescale and require transitions among different electronic states that violate the Born-Oppenheimer approximation (BOA). Non-BOA transitions pose challenges to both theory and experiment. From a theoretical point of view, excited state dynamics and nonadiabatic transitions both are difficult problems (see Figure 1(a)). However, the theory on non-BOA dynamics has advanced significantly over the last two decades. Full dynamical simulations for molecules of the size of nucleobases have been possible for a couple of years and allow predictions of experimental observables like photoelectron energy or ion yield. The availability of these calculations for isolated molecules has spurred new experimental efforts to develop methods that are sufficiently different from all optical techniques. For determination of transient molecular structure, femtosecond X-ray diffraction and electron diffraction have been implemented on optically excited molecules.
It is quite generally assumed that the overdamped Langevin equation provides a quantitative description of the dynamics of a classical Brownian particle in the long time limit. We establish and investigate a paradigm anomalous diffusion process governed by an underdamped Langevin equation with an explicit time dependence of the system temperature and thus the diffusion and damping coefficients. We show that for this underdamped scaled Brownian motion (UDSBM) the overdamped limit fails to describe the long time behaviour of the system and may practically even not exist at all for a certain range of the parameter values. Thus persistent inertial effects play a non-negligible role even at significantly long times. From this study a general questions on the applicability of the overdamped limit to describe the long time motion of an anomalously diffusing particle arises, with profound consequences for the relevance of overdamped anomalous diffusion models. We elucidate our results in view of analytical and simulations results for the anomalous diffusion of particles in free cooling granular gases.
It is quite generally assumed that the overdamped Langevin equation provides a quantitative description of the dynamics of a classical Brownian particle in the long time limit. We establish and investigate a paradigm anomalous diffusion process governed by an underdamped Langevin equation with an explicit time dependence of the system temperature and thus the diffusion and damping coefficients. We show that for this underdamped scaled Brownian motion (UDSBM) the overdamped limit fails to describe the long time behaviour of the system and may practically even not exist at all for a certain range of the parameter values. Thus persistent inertial effects play a non-negligible role even at significantly long times. From this study a general questions on the applicability of the overdamped limit to describe the long time motion of an anomalously diffusing particle arises, with profound consequences for the relevance of overdamped anomalous diffusion models. We elucidate our results in view of analytical and simulations results for the anomalous diffusion of particles in free cooling granular gases.
This publications-based thesis summarizes my contribution to the scientific field of ultrafast structural dynamics. It consists of 16 publications, about the generation, detection and coupling of coherent gigahertz longitudinal acoustic phonons, also called hypersonic waves. To generate such high frequency phonons, femtosecond near infrared laser pulses were used to heat nanostructures composed of perovskite oxides on an ultrashort timescale. As a consequence the heated regions of such a nanostructure expand and a high frequency acoustic phonon pulse is generated. To detect such coherent acoustic sound pulses I use ultrafast variants of optical Brillouin and x-ray scattering. Here an incident optical or x-ray photon is scattered by the excited sound wave in the sample. The scattered light intensity measures the occupation of the phonon modes.
The central part of this work is the investigation of coherent high amplitude phonon wave packets which can behave nonlinearly, quite similar to shallow water waves which show a steepening of wave fronts or solitons well known as tsunamis. Due to the high amplitude of the acoustic wave packets in the solid, the acoustic properties can change significantly in the vicinity of the sound pulse. This may lead to a shape change of the pulse. I have observed by time-resolved Brillouin scattering, that a single cycle hypersound pulse shows a wavefront steepening. I excited hypersound pulses with strain amplitudes until 1% which I have calibrated by ultrafast x-ray diffraction (UXRD).
On the basis of this first experiment we developed the idea of the nonlinear mixing of narrowband phonon wave packets which we call "nonlinear phononics" in analogy with the nonlinear optics, which summarizes a kaleidoscope of surprising optical phenomena showing up at very high electric fields. Such phenomena are for instance Second Harmonic Generation, four-wave-mixing or solitons. But in case of excited coherent phonons the wave packets have usually very broad spectra which make it nearly impossible to look at elementary scattering processes between phonons with certain momentum and energy.
For that purpose I tested different techniques to excite narrowband phonon wave packets which mainly consist of phonons with a certain momentum and frequency. To this end epitaxially grown metal films on a dielectric substrate were excited with a train of laser pulses. These excitation pulses drive the metal film to oscillate with the frequency given by their inverse temporal displacement and send a hypersonic wave of this frequency into the substrate. The monochromaticity of these wave packets was proven by ultrafast optical Brillouin and x-ray scattering.
Using the excitation of such narrowband phonon wave packets I was able to observe the Second Harmonic Generation (SHG) of coherent phonons as a first example of nonlinear wave mixing of nanometric phonon wave packets.
Gravity dictates the structure of the whole Universe and, although it is triumphantly described by the theory of General Relativity, it is the force that we least understand in nature. One of the cardinal predictions of this theory are black holes. Massive, dark objects are found in the majority of galaxies. Our own galactic center very contains such an object with a mass of about four million solar masses. Are these objects supermassive black holes (SMBHs), or do we need alternatives? The answer lies in the event horizon, the characteristic that defines a black hole. The key to probe the horizon is to model the movement of stars around a SMBH, and the interactions between them, and look for deviations from real observations. Nuclear star clusters harboring a massive, dark object with a mass of up to ~ ten million solar masses are good testbeds to probe the event horizon of the potential SMBH with stars. The channel for interactions between stars and the central MBH are the fact that (a) compact stars and stellar-mass black holes can gradually inspiral into the SMBH due to the emission of gravitational radiation, which is known as an “Extreme Mass Ratio Inspiral” (EMRI), and (b) stars can produce gases which will be accreted by the SMBH through normal stellar evolution, or by collisions and disruptions brought about by the strong central tidal field. Such processes can contribute significantly to the mass of the SMBH. These two processes involve different disciplines, which combined will provide us with detailed information about the fabric of space and time. In this habilitation I present nine articles of my recent work directly related with these topics.
We investigate the ensemble and time averaged mean squared displacements for particle diffusion in a simple model for disordered media by assuming that the local diffusivity is both fluctuating in time and has a deterministic average growth or decay in time. In this study we compare computer simulations of the stochastic Langevin equation for this random diffusion process with analytical results. We explore the regimes of normal Brownian motion as well as anomalous diffusion in the sub- and superdiffusive regimes. We also consider effects of the inertial term on the particle motion. The investigation of the resulting diffusion is performed for unconfined and confined motion.
We investigate the ensemble and time averaged mean squared displacements for particle diffusion in a simple model for disordered media by assuming that the local diffusivity is both fluctuating in time and has a deterministic average growth or decay in time. In this study we compare computer simulations of the stochastic Langevin equation for this random diffusion process with analytical results. We explore the regimes of normal Brownian motion as well as anomalous diffusion in the sub- and superdiffusive regimes. We also consider effects of the inertial term on the particle motion. The investigation of the resulting diffusion is performed for unconfined and confined motion.
What are the physical laws of the mutual interactions of objects bound to cell membranes, such as various membrane proteins or elongated virus particles? To rationalise this, we here investigate by extensive computer simulations mutual interactions of rod-like particles adsorbed on the surface of responsive elastic two-dimensional sheets. Specifically, we quantify sheet deformations as a response to adhesion of such filamentous particles. We demonstrate that tip-to-tip contacts of rods are favoured for relatively soft sheets, while side-by-side contacts are preferred for stiffer elastic substrates. These attractive orientation-dependent substrate-mediated interactions between the rod-like particles on responsive sheets can drive their aggregation and self-assembly. The optimal orientation of the membrane-bound rods is established via responding to the elastic energy profiles created around the particles. We unveil the phase diagramme of attractive–repulsive rod–rod interactions in the plane of their separation and mutual orientation. Applications of our results to other systems featuring membrane-associated particles are also discussed.
What are the physical laws of the mutual interactions of objects bound to cell membranes, such as various membrane proteins or elongated virus particles? To rationalise this, we here investigate by extensive computer simulations mutual interactions of rod-like particles adsorbed on the surface of responsive elastic two-dimensional sheets. Specifically, we quantify sheet deformations as a response to adhesion of such filamentous particles. We demonstrate that tip-to-tip contacts of rods are favoured for relatively soft sheets, while side-by-side contacts are preferred for stiffer elastic substrates. These attractive orientation-dependent substrate-mediated interactions between the rod-like particles on responsive sheets can drive their aggregation and self-assembly. The optimal orientation of the membrane-bound rods is established via responding to the elastic energy profiles created around the particles. We unveil the phase diagramme of attractive–repulsive rod–rod interactions in the plane of their separation and mutual orientation. Applications of our results to other systems featuring membrane-associated particles are also discussed.
Changes in extratropical storm track activity and their implications for extreme weather events
(2016)
In this thesis, the two prototype catalysts Fe(CO)₅ and Cr(CO)₆ are investigated with time-resolved photoelectron spectroscopy at a high harmonic setup. In both of these metal carbonyls, a UV photon can induce the dissociation of one or more ligands of the complex. The mechanism of the dissociation has been debated over the last decades. The electronic dynamics of the first dissociation occur on the femtosecond timescale.
For the experiment, an existing high harmonic setup was moved to a new location, was extended, and characterized. The modified setup can induce dynamics in gas phase samples with photon energies of 1.55eV, 3.10eV, and 4.65eV. The valence electronic structure of the samples can be probed with photon energies between 20eV and 40eV. The temporal resolution is 111fs to 262fs, depending on the combination of the two photon energies.
The electronically excited intermediates of the two complexes, as well as of the reaction product Fe(CO)₄, could be observed with photoelectron spectroscopy in the gas phase for the first time. However, photoelectron spectroscopy gives access only to the final ionic states. Corresponding calculations to simulate these spectra are still in development. The peak energies and their evolution in time with respect to the initiation pump pulse have been determined, these peaks have been assigned based on literature data. The spectra of the two complexes show clear differences. The dynamics have been interpreted with the assumption that the motion of peaks in the spectra relates to the movement of the wave packet in the multidimensional energy landscape. The results largely confirm existing models for the reaction pathways. In both metal carbonyls, this pathway involves a direct excitation of the wave packet to a metal-to-ligand charge transfer state and the subsequent crossing to a dissociative ligand field state. The coupling of the electronic dynamics to the nuclear dynamics could explain the slower dissociation in Fe(CO)₅ as compared to Cr(CO)₆.
The cell interior is a highly packed environment in which biological macromolecules evolve and function. This crowded media has effects in many biological processes such as protein-protein binding, gene regulation, and protein folding. Thus, biochemical reactions that take place in such crowded conditions differ from diluted test tube conditions, and a considerable effort has been invested in order to understand such differences.
In this work, we combine different computationally tools to disentangle the effects of molecular crowding on biochemical processes. First, we propose a lattice model to study the implications of molecular crowding on enzymatic reactions. We provide a detailed picture of how crowding affects binding and unbinding events and how the separate effects of crowding on binding equilibrium act together. Then, we implement a lattice model to study the effects of molecular crowding on facilitated diffusion. We find that obstacles on the DNA impair facilitated diffusion. However, the extent of this effect depends on how dynamic obstacles are on the DNA. For the scenario in which crowders are only present in the bulk solution, we find that at some conditions presence of crowding agents can enhance specific-DNA binding. Finally, we make use of structure-based techniques to look at the impact of the presence of crowders on the folding a protein. We find that polymeric crowders have stronger effects on protein stability than spherical crowders. The strength of this effect increases as the polymeric crowders become longer. The methods we propose here are general and can also be applied to more complicated systems.