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Auger-photoelectron coincidence spectroscopy (APECS) has been used to examine the electron correlation and itinerance effects in transition metals Cu, Ni and Co.
It is shown that the LVV Auger, in coincidence with 2p photoelectrons, spectra can be represented using atomic multiplet positions if the 3d-shell is localized (atomic-like) and with a self-convoluted valence band for band-like (itinerant) materials as explained using the Cini-Sawatzky model.
For transition metals, the 3d band changes from band-like to localized with increasing atomic number, with the possibility of a mixed behavior.
Our result shows that the LVV spectra of Cu can be represented by atomic multiplet calculations, those of Co resemble the self-convolution of the valence band and those of Ni are a mixture of both, consistent with the Cini-Sawatzky model.
Porous ceramic diesel particulate filters (DPFs) are extruded products that possess macroscopic anisotropic mechanical and thermal properties. This anisotropy is caused by both morphological features (mostly the orientation of porosity) and crystallographic texture. We systematically studied those two aspects in two aluminum titanate ceramic materials of different porosity using mercury porosimetry, gas adsorption, electron microscopy, X-ray diffraction, and X-ray refraction radiography. We found that a lower porosity content implies a larger isotropy of both the crystal texture and the porosity orientation. We also found that, analogous to cordierite, crystallites do align with their axis of negative thermal expansion along the extrusion direction. However, unlike what found for cordierite, the aluminium titanate crystallite form is such that a more pronounced (0 0 2) texture along the extrusion direction implies porosity aligned perpendicular to it.
SwSt 1 (PN G001.5-06.7) is a bright and compact planetary nebula containing a late [WC]-type central star. Previous studies suggested that the nebular and stellar lines are slowly changing with time. We studied new and archival optical and ultraviolet spectra of the object. The [O III] 4959 and 5007 angstrom to H beta line flux ratios decreased between about 1976 and 1997/2015. The stellar spectrum also shows changes between these epochs. We modelled the stellar and nebular spectra observed at different epochs. The analyses indicate a drop of the stellar temperature from about 42 kK to 40.5 kK between 1976 and 1993. We do not detect significant changes between 1993 and 2015. The observations show that the star performed a loop in the H-R diagram. This is possible when a shell source is activated during its post-AGB evolution. We infer that a late thermal pulse (LTP) experienced by a massive post-AGB star can explain the evolution of the central star. Such a star does not expand significantly as the result of the LTP and does not became a born-again red giant. However, the released energy can remove the tiny H envelope of the star.
In normal everyday viewing, we perform large eye movements (saccades) and miniature or fixational eye movements. Most of our visual perception occurs while we are fixating. However, our eyes are perpetually in motion. Properties of these fixational eye movements, which are partly controlled by the brainstem, change depending on the task and the visual conditions. Currently, fixational eye movements are poorly understood because they serve the two contradictory functions of gaze stabilization and counteraction of retinal fatigue. In this dissertation, we investigate the spatial and temporal properties of time series of eye position acquired from participants staring at a tiny fixation dot or at a completely dark screen (with the instruction to fixate a remembered stimulus); these time series were acquired with high spatial and temporal resolution. First, we suggest an advanced algorithm to separate the slow phases (named drift) and fast phases (named microsaccades) of these movements, which are considered to play different roles in perception. On the basis of this identification, we investigate and compare the temporal scaling properties of the complete time series and those time series where the microsaccades are removed. For the time series obtained during fixations on a stimulus, we were able to show that they deviate from Brownian motion. On short time scales, eye movements are governed by persistent behavior and on a longer time scales, by anti-persistent behavior. The crossover point between these two regimes remains unchanged by the removal of microsaccades but is different in the horizontal and the vertical components of the eyes. Other analyses target the properties of the microsaccades, e.g., the rate and amplitude distributions, and we investigate, whether microsaccades are triggered dynamically, as a result of earlier events in the drift, or completely randomly. The results obtained from using a simple box-count measure contradict the hypothesis of a purely random generation of microsaccades (Poisson process). Second, we set up a model for the slow part of the fixational eye movements. The model is based on a delayed random walk approach within the velocity related equation, which allows us to use the data to determine control loop durations; these durations appear to be different for the vertical and horizontal components of the eye movements. The model is also motivated by the known physiological representation of saccade generation; the difference between horizontal and vertical components concurs with the spatially separated representation of saccade generating regions. Furthermore, the control loop durations in the model suggest an external feedback loop for the horizontal but not for the vertical component, which is consistent with the fact that an internal feedback loop in the neurophysiology has only been identified for the vertical component. Finally, we confirmed the scaling properties of the model by semi-analytical calculations. In conclusion, we were able to identify several properties of the different parts of fixational eye movements and propose a model approach that is in accordance with the described neurophysiology and described limitations of fixational eye movement control.
The Bow on a String
(2018)
The interaction between a bowed string instrument and its player is conveyed by the bow, the vibrational properties of which can be measured either separately on the bow or during the bowing procedure. Here, two piezoelectric film sensors, made of a ferroelectret material, are installed on a violin bow, one sensor at the tip and one at the frog. With these sensors, a violin is played under normal conditions, and the signals are analysed. The features in the resulting spectrograms are identified as string harmonics and longitudinal bow-hair resonances. The bow-hair sections on both sides of the bow-string contact exhibit separate resonances which are observed as absorption dips in the spectra. Owing to the sensor positions at the bow-hair terminations, it can be inferred that the two bow-hair sections act as mutual vibration absorbers. From a regression of the observed resonances, the longitudinal bow-hair velocity can be obtained. With additional film sensors under the violin bridge, body vibrations were also detected providing further details of the coupling mechanisms.
The Sun’s atmosphere is frequently disrupted by coronal mass ejections (CMEs), coupled with flares and energetic particles. The coupling is usually attributed to magnetic reconnection at a vertical current sheet connecting the flare and CME, with the latter embedding a helical magnetic structure known as flux rope. However, both the origin of flux ropes and their nascent paths toward eruption remain elusive. Here, we present an observation of how a stellar-sized CME bubble evolves continuously from plasmoids, mini flux ropes that are barely resolved, within half an hour. The eruption initiates when plasmoids springing from a vertical current sheet merge into a leading plasmoid, which rises at increasing speeds and expands impulsively into the CME bubble, producing hard x-ray bursts simultaneously. This observation illuminates a complete CME evolutionary path capable of accommodating a wide variety of plasma phenomena by bridging the gap between microscale and macroscale dynamics.
During the last few years there was a tremendous growth of scientific activities in the fields related to both Physics and Control theory: nonlinear dynamics, micro- and nanotechnologies, self-organization and complexity, etc. New horizons were opened and new exciting applications emerged. Experts with different backgrounds starting to work together need more opportunities for information exchange to improve mutual understanding and cooperation. The Conference "Physics and Control 2007" is the third international conference focusing on the borderland between Physics and Control with emphasis on both theory and applications. With its 2007 address at Potsdam, Germany, the conference is located for the first time outside of Russia. The major goal of the Conference is to bring together researchers from different scientific communities and to gain some general and unified perspectives in the studies of controlled systems in physics, engineering, chemistry, biology and other natural sciences. We hope that the Conference helps experts in control theory to get acquainted with new interesting problems, and helps experts in physics and related fields to know more about ideas and tools from the modern control theory.
The blazar Mrk 501 (z = 0.034) was observed at very-high-energy (VHE, E greater than or similar to 100 GeV) gamma-ray wavelengths during a bright flare on the night of 2014 June 23-24 (MJD 56832) with the H.E.S.S. phase-II array of Cherenkov telescopes. Data taken that night by H.E.S.S. at large zenith angle reveal an exceptional number of gamma-ray photons at multi-TeV energies, with rapid flux variability and an energy coverage extending significantly up to 20 TeV. This data set is used to constrain Lorentz invariance violation (LIV) using two independent channels: a temporal approach considers the possibility of an energy dependence in the arrival time of gamma-rays, whereas a spectral approach considers the possibility of modifications to the interaction of VHE gamma-rays with extragalactic background light (EBL) photons. The non-detection of energy-dependent time delays and the non-observation of deviations between the measured spectrum and that of a supposed power-law intrinsic spectrum with standard EBL attenuation are used independently to derive strong constraints on the energy scale of LIV (E-QG) in the subluminal scenario for linear and quadratic perturbations in the dispersion relation of photons. For the case of linear perturbations, the 95% confidence level limits obtained are E-QG,E-1 > 3.6 x 10(17) GeV using the temporal approach and E-QG,E-1 > 2.6 x 10(19) GeV using the spectral approach. For the case of quadratic perturbations, the limits obtained are E-QG,E-2 > 8.5 x 10(10) GeV using the temporal approach and E-QG,E-2 > 7.8 x 10(11) GeV using the spectral approach.
We review the evidence for a putative early 21st-century divergence between global mean surface temperature (GMST) and Coupled Model Intercomparison Project Phase 5 (CMIP5) projections. We provide a systematic comparison between temperatures and projections using historical versions of GMST products and historical versions of model projections that existed at the times when claims about a divergence were made. The comparisons are conducted with a variety of statistical techniques that correct for problems in previous work, including using continuous trends and a Monte Carlo approach to simulate internal variability. The results show that there is no robust statistical evidence for a divergence between models and observations. The impression of a divergence early in the 21st century was caused by various biases in model interpretation and in the observations, and was unsupported by robust statistics.
As VLSI design moves into ultra-deep-submicron technologies, timing margins added to the clock period are mandatory, to ensure correct circuit behavior under worst-case conditions. Timing resilient architectures emerged as a promising solution to alleviate these worst-case timing margins. These architectures allow improving system performance and reducing energy consumption. Asynchronous systems, on the other hand, have the potential to improve energy efficiency and performance. Blade is an asynchronous timing resilient template that leverages the advantages of both asynchronous and timing resilient techniques. However, Blade still presents challenges regarding its testability, which hinders its commercial or large-scale application. This paper demonstrates that scan chains can be prohibitive for Blade due to their high silicon costs., which can reach more than 100%. Then, it proposes an alternative test approach that allows concurrent testing, stuck-at, and delay testing. The test approach is based on the reuse the Blade features to provide testability, with silicon area overheads between 4 and 7%.
Context.
The supergiant ionized shell SMC-SGS 1 (DEM 167), which is located in the outer Wing of the Small Magellanic Cloud (SMC), resembles structures that originate from an energetic star-formation event and later stimulate star formation as they expand into the ambient medium. However, stellar populations within and surrounding SMC-SGS 1 tell a different story. Aims. We present a photometric study of the stellar population encompassed by SMC-SGS 1 in order to trace the history of such a large structure and its potential influence on star formation within the low-density, low-metallicity environment of the SMC.
Methods.
For a stellar population that is physically associated with SMC-SGS 1, we combined near-ultraviolet (NUV) photometry from the Galaxy Evolution Explorer with archival optical (V-band) photometry from the ESO Danish 1.54 m Telescope. Given their colors and luminosities, we estimated stellar ages and masses by matching observed photometry to theoretical stellar isochrone models. Results. We find that the investigated region supports an active, extended star-formation event spanning similar to 25-40 Myr ago, as well as continued star formation into the present. Using a standard initial mass function, we infer a lower bound on the stellar mass from this period of similar to 3 x 10(4) M-circle dot, corresponding to a star-formation intensity of similar to 6 x 10(-3) M-circle dot kpc(-2) yr(-1).
Conclusions.
The spatial and temporal distributions of young stars encompassed by SMC-SGS 1 imply a slow, consistent progression of star formation over millions of years. Ongoing star formation, both along the edge and interior to SMC-SGS 1, suggests a combined stimulated and stochastic mode of star formation within the SMC Wing. We note that a slow expansion of the shell within this low-density environment may preserve molecular clouds within the volume of the shell, leaving them to form stars even after nearby stellar feedback expels local gas and dust.
We present different tests for phase synchronization which improve the procedures currently used in the literature. This is accomplished by using a two-samples test setup and by utilizing insights and methods from directional statistics and bootstrap theory. The tests differ in the generality of the situation in which they can be applied as well as in their complexity, including computational cost. A modification of the resampling technique of the bootstrap is introduced, making it possible to fully utilize data from time series.
Tensorial spacetime geometries carrying predictive, interpretable and quantizable matter dynamics
(2012)
Which tensor fields G on a smooth manifold M can serve as a spacetime structure? In the first part of this thesis, it is found that only a severely restricted class of tensor fields can provide classical spacetime geometries, namely those that can carry predictive, interpretable and quantizable matter dynamics. The obvious dependence of this characterization of admissible tensorial spacetime geometries on specific matter is not a weakness, but rather presents an insight: it was Maxwell theory that justified Einstein to promote Lorentzian manifolds to the status of a spacetime geometry. Any matter that does not mimick the structure of Maxwell theory, will force us to choose another geometry on which the matter dynamics of interest are predictive, interpretable and quantizable. These three physical conditions on matter impose three corresponding algebraic conditions on the totally symmetric contravariant coefficient tensor field P that determines the principal symbol of the matter field equations in terms of the geometric tensor G: the tensor field P must be hyperbolic, time-orientable and energy-distinguishing. Remarkably, these physically necessary conditions on the geometry are mathematically already sufficient to realize all kinematical constructions familiar from Lorentzian geometry, for precisely the same structural reasons. This we were able to show employing a subtle interplay of convex analysis, the theory of partial differential equations and real algebraic geometry. In the second part of this thesis, we then explore general properties of any hyperbolic, time-orientable and energy-distinguishing tensorial geometry. Physically most important are the construction of freely falling non-rotating laboratories, the appearance of admissible modified dispersion relations to particular observers, and the identification of a mechanism that explains why massive particles that are faster than some massless particles can radiate off energy until they are slower than all massless particles in any hyperbolic, time-orientable and energy-distinguishing geometry. In the third part of the thesis, we explore how tensorial spacetime geometries fare when one wants to quantize particles and fields on them. This study is motivated, in part, in order to provide the tools to calculate the rate at which superluminal particles radiate off energy to become infraluminal, as explained above. Remarkably, it is again the three geometric conditions of hyperbolicity, time-orientability and energy-distinguishability that allow the quantization of general linear electrodynamics on an area metric spacetime and the quantization of massive point particles obeying any admissible dispersion relation. We explore the issue of field equations of all possible derivative order in rather systematic fashion, and prove a practically most useful theorem that determines Dirac algebras allowing the reduction of derivative orders. The final part of the thesis presents the sketch of a truly remarkable result that was obtained building on the work of the present thesis. Particularly based on the subtle duality maps between momenta and velocities in general tensorial spacetimes, it could be shown that gravitational dynamics for hyperbolic, time-orientable and energy distinguishable geometries need not be postulated, but the formidable physical problem of their construction can be reduced to a mere mathematical task: the solution of a system of homogeneous linear partial differential equations. This far-reaching physical result on modified gravity theories is a direct, but difficult to derive, outcome of the findings in the present thesis. Throughout the thesis, the abstract theory is illustrated through instructive examples.
Famously, Einstein read off the geometry of spacetime from Maxwell's equations. Today, we take this geometry that serious that our fundamental theory of matter, the standard model of particle physics, is based on it. However, it seems that there is a gap in our understanding if it comes to the physics outside of the solar system. Independent surveys show that we need concepts like dark matter and dark energy to make our models fit with the observations. But these concepts do not fit in the standard model of particle physics. To overcome this problem, at least, we have to be open to matter fields with kinematics and dynamics beyond the standard model. But these matter fields might then very well correspond to different spacetime geometries. This is the basis of this thesis: it studies the underlying spacetime geometries and ventures into the quantization of those matter fields independently of any background geometry. In the first part of this thesis, conditions are identified that a general tensorial geometry must fulfill to serve as a viable spacetime structure. Kinematics of massless and massive point particles on such geometries are introduced and the physical implications are investigated. Additionally, field equations for massive matter fields are constructed like for example a modified Dirac equation. In the second part, a background independent formulation of quantum field theory, the general boundary formulation, is reviewed. The general boundary formulation is then applied to the Unruh effect as a testing ground and first attempts are made to quantize massive matter fields on tensorial spacetimes.
Mechanosensation is a fundamental biological process that provides the basis for sensing touch and pain as well as for hearing and proprioception. A special class of ion-channel proteins known as mechanosensitive proteins convert the mechanical stimuli into electrochemical signals to mediate this process. Mechanosensitive proteins undergo conformational changes in response to mechanical force, which eventually leads to the opening of the proteins' ion channel. Mammalian mechanosensitive proteins remained a long sought-after mystery until 2010 when a family of two proteins - Piezo1 and Piezo2 - was identifed as mechanosensors [1]. The cryo-EM structures of Piezo1 and Piezo2 protein were resolved in the last years and reveal a propeller-shaped homotrimer with 114 transmembrane helices [2, 3, 4, 5]. The protein structures are curved and have been suggested to deform the surrounding membrane into a nano-dome, which mechanically responds to membrane tension resulting from external forces [2]. In this thesis, the conformations of membrane-embedded Piezo1 and Piezo2 proteins and their tension-induced conformational changes are investigated using molecular dynamics simulations. Our coarse-grained molecular dynamics simulations show that the Piezo proteins induce curvature in the surrounding membrane and form a stable protein-membrane nano-dome in the tensionless membrane. These membrane-embedded Piezo proteins, however, adopt substantially less curved conformations in our simulations compared to the cryo-EM structures solved in detergent micelles, which agrees with recent experimental investigations of the overall Piezo nano-dome shape in membrane vesicles [6, 7, 8]. At high membrane tension, the Piezo proteins attain nearly planar conformations in our simulations. Our systematic investigation of Piezo proteins under different membrane tensions indicates a half-maximal conformational response at membrane tension values rather close to the experimentally suggested values of Piezo activation [9, 10]. In addition, our simulations indicate a widening of the Piezo1 ion channel at high membrane tension, which agrees with the channel widening observed in recent nearly flattened cryo-EM structures of Piezo1 in small membrane vesicles [11]. In contrast, the Piezo2 ion channel does not respond to membrane tension in our simulations. These different responses of the Piezo1 and Piezo2 ion channels in our simulations are in line with patch-clamp experiments, in which Piezo1, but not Piezo2, was shown to be activated by membrane tension alone [12].
We investigate the cognitive control in polyrhythmic hand movements as a model paradigm for bimanual coordination. Using a symbolic coding of the recorded time series, we demonstrate the existence of qualitative transitions induced by experimental manipulation of the tempo. A nonlinear model with delayed feedback control is proposed, which accounts for these dynamical transitions in terms of bifurcations resulting from variation of the external control parameter. Furthermore, it is shown that transitions can also be observed due to fluctuations in the timing control level. We conclude that the complexity of coordinated bimanual movements results from interactions between nonlinear control mechanisms with delayed feedback and stochastic timing components.
In ferroelectrets, the piezoelectricity stems from the charges of both polarities trapped on the inner surfaces of the cavities in the material, so that its thermal stability is defined by the stability of the respective charges. In the present work, a template-based lamination technique has been employed to fabricate tubular-channel ferroelectrets from fluoroethylenepropylene (FEP) films. It has been shown that the piezoelectricity in FEP ferroelectrets decays at relatively low temperatures due to the inherently lower thermal stability of the positive charge. In order to improve charge trapping, we have treated both FEP films and inner surfaces of the ferroelectret cavities with titanium-tetrachloride vapor, using the atomic-layer-deposition technique. Using surface-potential-decay measurements on FEP films, we have found that the charge-decay curves shift by more than 100 degrees C to the higher temperatures as a result of the surface treatment. Direct measurements of piezoelectric d(33) coefficients as a function of temperature have shown that the piezoelectric stability is likewise improved with the d(33)-decay curves shifted by 60 degrees C to the right. The improvement of electret/ferroelectret properties can be attributed to the formation of the deeper traps on the chemically modified FEP surface. SEM micrographs and EDS analysis reveal island-like structures with titanium- and oxygen-containing species that can be responsible for the deeper trapping of the electret charges. Published by AIP Publishing.
Solvent vapor annealing is as an effective and versatile alternative to thermal annealing to equilibrate and control the assembly of polymer chains in thin films. Here, we present scientific and practical aspects of the solvent vapor annealing method, including the discussion of such factors as non-equilibrium conformational states and chain dynamics in thin films in the presence of solvent. Homopolymer and block copolymer films have been used in model studies to evaluate the robustness and the reproducibility of the solvent vapor processing, as well as to assess polymer-solvent interactions under confinement. Advantages of utilizing a well-controlled solvent vapor environment, including practically interesting regimes of weakly saturated vapor leading to poorly swollen states, are discussed. Special focus is given to dual temperature control over the set-up instrumentation and to the potential of solvo-thermal annealing. The evaluated insights into annealing dynamics derived from the studies on block copolymer films can be applied to improve the processing of thin films of crystalline and conjugated polymers as well as polymer composite in confined geometries.
Tautomerism is one of the most important forms of isomerism, owing to the facile interconversion between species and the large differences in chemical properties introduced by the proton transfer connecting the tautomers. Spectroscopic techniques are often used for the characterization of tautomers. In this context, separating the overlapping spectral response of coexisting tautomers is a long-standing challenge in chemistry. Here, we demonstrate that by using resonant inelastic X-ray scattering tuned to the core excited states at the site of proton exchange between tautomers one is able to experimentally disentangle the manifold of valence excited states of each tautomer in a mixture. The technique is applied to the prototypical keto-enol equilibrium of 3-hydroxypyridine in aqueous solution. We detect transitions from the occupied orbitals into the LUMO for each tautomer in solution, which report on intrinsic and hydrogen-bond-induced orbital polarization within the pi and sigma manifolds at the proton-transfer site.
A huge number of applications require coherent radiation in the visible spectral range. Since diode lasers are very compact and efficient light sources, there exists a great interest to cover these applications with diode laser emission. Despite modern band gap engineering not all wavelengths can be accessed with diode laser radiation. Especially in the visible spectral range between 480 nm and 630 nm no emission from diode lasers is available, yet. Nonlinear frequency conversion of near-infrared radiation is a common way to generate coherent emission in the visible spectral range. However, radiation with extraordinary spatial temporal and spectral quality is required to pump frequency conversion. Broad area (BA) diode lasers are reliable high power light sources in the near-infrared spectral range. They belong to the most efficient coherent light sources with electro-optical efficiencies of more than 70%. Standard BA lasers are not suitable as pump lasers for frequency conversion because of their poor beam quality and spectral properties. For this purpose, tapered lasers and diode lasers with Bragg gratings are utilized. However, these new diode laser structures demand for additional manufacturing and assembling steps that makes their processing challenging and expensive. An alternative to BA diode lasers is the stripe-array architecture. The emitting area of a stripe-array diode laser is comparable to a BA device and the manufacturing of these arrays requires only one additional process step. Such a stripe-array consists of several narrow striped emitters realized with close proximity. Due to the overlap of the fields of neighboring emitters or the presence of leaky waves, a strong coupling between the emitters exists. As a consequence, the emission of such an array is characterized by a so called supermode. However, for the free running stripe-array mode competition between several supermodes occurs because of the lack of wavelength stabilization. This leads to power fluctuations, spectral instabilities and poor beam quality. Thus, it was necessary to study the emission properties of those stripe-arrays to find new concepts to realize an external synchronization of the emitters. The aim was to achieve stable longitudinal and transversal single mode operation with high output powers giving a brightness sufficient for efficient nonlinear frequency conversion. For this purpose a comprehensive analysis of the stripe-array devices was done here. The physical effects that are the origin of the emission characteristics were investigated theoretically and experimentally. In this context numerical models could be verified and extended. A good agreement between simulation and experiment was observed. One way to stabilize a specific supermode of an array is to operate it in an external cavity. Based on mathematical simulations and experimental work, it was possible to design novel external cavities to select a specific supermode and stabilize all emitters of the array at the same wavelength. This resulted in stable emission with 1 W output power, a narrow bandwidth in the range of 2 MHz and a very good beam quality with M²<1.5. This is a new level of brightness and brilliance compared to other BA and stripe-array diode laser systems. The emission from this external cavity diode laser (ECDL) satisfied the requirements for nonlinear frequency conversion. Furthermore, a huge improvement to existing concepts was made. In the next step newly available periodically poled crystals were used for second harmonic generation (SHG) in single pass setups. With the stripe-array ECDL as pump source, more than 140 mW of coherent radiation at 488 nm could be generated with a very high opto-optical conversion efficiency. The generated blue light had very good transversal and longitudinal properties and could be used to generate biphotons by parametric down-conversion. This was feasible because of the improvement made with the infrared stripe-array diode lasers due to the development of new physical concepts.
Poly(vinylidene fluoride) (PVDF)-based homo-, co- and ter-polymers are well-known for their ferroelectric and relaxor-ferroelectric properties. Their semi-crystalline morphology consists of crystalline and amorphous phases, plus interface regions in between, and governs the relevant electro-active properties. In this work, the influence of chemical, thermal and mechanical treatments on the structure and morphology of PVDF-based polymers and on the related ferroelectric/relaxor-ferroelectric properties is investigated. Polymer films were prepared in different ways and subjected to various treatments such as annealing, quenching and stretching. The resulting changes in the transitions and relaxations of the polymer samples were studied by means of dielectric, thermal, mechanical and optical techniques. In particular, the origin(s) behind the mysterious mid-temperature transition (T_{mid}) that is observed in all PVDF-based polymers was assessed. A new hypothesis is proposed to describe the T_{mid} transition as a result of multiple processes taking place within the temperature range of the transition. The contribution of the individual processes to the observed overall transition depends on both the chemical structure of the monomer units and the processing conditions which also affect the melting transition. Quenching results in a decrease of the overall crystallinity and in smaller crystallites. On samples quenched after annealing, notable differences in the fractions of different crystalline phases have been observed when compared to samples that had been slowly cooled. Stretching of poly(vinylidene fluoride-tetrafluoroethylene) (P(VDF-TFE)) films causes an increase in the fraction of the ferroelectric β-phase with simultaneous increments in the melting point (T_m) and the crystallinity (\chi_c) of the copolymer. While an increase in the stretching temperature does not have a profound effect on the amount of the ferroelectric phase, its stability appears to improve.
Measurements of the non-linear dielectric permittivity \varepsilon_2^\prime in a poly(vinylidenefluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE- CFE)) relaxor-ferroelectric (R-F) terpolymer reveal peaks at 30 and 80 °C that cannot be identified in conventional dielectric spectroscopy. The former peak is associated with T_{mid}\ and may help to understand the non-zero \varepsilon_2^\prime values that are found for the paraelectric terpolymer phase. The latter peak can also be observed during cooling of P(VDF-TrFE) copolymer samples at 100 °C and is due to conduction processes and space-charge polarization as a result of the accumulation of real charges at the electrode-sample interface. Annealing lowers the Curie-transition temperature of the terpolymer as a consequence of its smaller ferroelectric-phase fraction, which by default exists even in terpolymers with relatively high CFE content. Changes in the transition temperatures are in turn related to the behavior of the hysteresis curves observed on differently heat-treated samples. Upon heating, the hysteresis curves evolve from those known for a ferroelectric to those of a typical relaxor-ferroelectric material. Comparing dielectric-hysteresis loops obtained at various temperatures, we find that annealed terpolymer films show higher electric-displacement values and lower coercive fields than the non-annealed samples − irrespective of the measurement temperature − and also exhibit ideal relaxor-ferroelectric behavior at ambient temperatures, which makes them excellent candidates for related applications at or near room temperature. However, non-annealed films − by virtue of their higher ferroelectric activity − show a larger and more stable remanent polarization at room temperature, while annealed samples need to be poled below 0 °C to induce a well-defined polarization. Overall, by modifying the three phases in PVDF-based polymers, it has been demonstrated how the preparation steps and processing conditions can be tailored to achieve the desired properties that are optimal for specific applications.
Excited-state proton transfer (ESPT) is a fundamental process in biomolecular photochemistry, but its underlying mediators often evade direct observation. We identify a distinct pathway for ESPT in aqueous 2-thiopyridone, by employing transient N1s X-ray absorption spectroscopy and multi-configurational spectrum simulations. Photoexcitations to the singlet S-2 and S-4 states both relax promptly through intersystem crossing to the triplet T-1 state. The T-1 state, through its rapid population and near nanosecond lifetime, mediates nitrogen site deprotonation by ESPT in a secondary intersystem crossing to the S-0 potential energy surface. This conclusively establishes a dominant ESPT pathway for the system in aqueous solution, which is also compatible with previous measurements in acetonitrile. Thereby, the hitherto open questions of the pathway for ESPT in the compound, including its possible dependence on excitation wavelength and choice of solvent, are resolved.
Context. Runaway stars form bow shocks by ploughing through the interstellar medium at supersonic speeds and are promising sources of non-thermal emission of photons. One of these objects has been found to emit non-thermal radiation in the radio band. This triggered the development of theoretical models predicting non-thermal photons from radio up to very-high-energy (VHE, E >= 0.1 TeV) gamma rays. Subsequently, one bow shock was also detected in X-ray observations. However, the data did not allow discrimination between a hot thermal and a non-thermal origin. Further observations of different candidates at X-ray energies showed no evidence for emission at the position of the bow shocks either. A systematic search in the Fermi-LAT energy regime resulted in flux upper limits for 27 candidates listed in the E-BOSS catalogue. Aims. Here we perform the first systematic search for VHE gamma-ray emission from bow shocks of runaway stars. Methods. Using all available archival H.E.S.S. data we search for very-high-energy gamma-ray emission at the positions of bow shock candidates listed in the second E-BOSS catalogue release. Out of the 73 bow shock candidates in this catalogue, 32 have been observed with H.E.S.S. Results. None of the observed 32 bow shock candidates in this population study show significant emission in the H.E.S.S. energy range. Therefore, flux upper limits are calculated in five energy bins and the fraction of the kinetic wind power that is converted into VHE gamma rays is constrained. Conclusions. Emission from stellar bow shocks is not detected in the energy range between 0.14 and 18 TeV. The resulting upper limits constrain the level of VHE gamma-ray emission from these objects down to 0.1-1% of the kinetic wind energy.
New amphiphilic compounds 1-9 that feature a construction with dendronized hydrophilic and hydrophobic segment groups connected to a specific aromatic or aliphatic spacer unit have been synthesized, following a modular building block strategy. The hydrophilic dendrons are typically branched elements with peripheral carboxylic groups, unlike the hydrophobic dendrons that contain peripheral alkyl chains as part of respective amide functions. The hydrophilic dendrons are in different generations of branching, while the hydrophobic dendrons are all in the first generation of branching (three terminal branching), but differ in the length of the alkyl chains, thus giving rise to designed structure and amphiphilic properties in the new compounds. The resulting surfactants are capable of forming well-defined Langmuir films of remarkable stability when spread from a solution onto an aqueous subphase. Nevertheless, specific packing behaviour and orientation of the amphiphilic molecules were found, depending on the molecular structure, as determined using analysis of the surface pressure-area (pi-A) isotherms. Langmuir-Blodgett transfer of the first monolayer from a pure water subphase to a clean silicon wafer proved possible for the amphiphiles of peripheral alkyl chain length C-12, while the amphiphiles with the longer alkyl chains failed, possibly due to the more rigid monolayers they form, impeding the transfer.
Synchrotron-based angle-resolved time-of-flight electron spectroscopy for dynamics in dichalogenides
(2018)
We consider collective dynamics in the ensemble of serially connected spin-torque oscillators governed by the Landau-Lifshitz-Gilbert-Slonczewski magnetization equation. Proximity to homoclinicity hampers synchronization of spin-torque oscillators: when the synchronous ensemble experiences the homoclinic bifurcation, the growth rate per oscillation of small deviations from the ensemble mean diverges. Depending on the configuration of the contour, sufficiently strong common noise, exemplified by stochastic oscillations of the current through the circuit, may suppress precession of the magnetic field for all oscillators. We derive the explicit expression for the threshold amplitude of noise, enabling this suppression.
<img src="http://vg00.met.vgwort.de/na/806c85cec18906a64e06" width="1" height="1" alt=""> Subject of this work is the possibility to synchronize nonlinear systems via correlated noise and automatic control. The thesis is divided into two parts. The first part is motivated by field studies on feral sheep populations on two islands of the St. Kilda archipelago, which revealed strong correlations due to environmental noise. For a linear system the population correlation equals the noise correlation (Moran effect). But there exists no systematic examination of the properties of nonlinear maps under the influence of correlated noise. Therefore, in the first part of this thesis the noise-induced correlation of logistic maps is systematically examined. For small noise intensities it can be shown analytically that the correlation of quadratic maps in the fixed-point regime is always smaller than or equal to the noise correlation. In the period-2 regime a Markov model explains qualitatively the main dynamical characteristics. Furthermore, two different mechanisms are introduced which lead to a higher correlation of the systems than the environmental correlation. The new effect of "correlation resonance" is described, i. e. the correlation yields a maximum depending on the noise intensity. In the second part of the thesis an automatic control method is presented which synchronizes different systems in a robust way. This method is inspired by phase-locked loops and is based on a feedback loop with a differential control scheme, which allows to change the phases of the controlled systems. The effectiveness of the approach is demonstrated for controlled phase synchronization of regular oscillators and foodweb models.
Subject of this work is the investigation of generic synchronization phenomena in interacting complex systems. These phenomena are observed, among all, in coupled deterministic chaotic systems. At very weak interactions between individual systems a transition to a weakly coherent behavior of the systems can take place. In coupled continuous time chaotic systems this transition manifests itself with the effect of phase synchronization, in coupled chaotic discrete time systems with the effect of non-vanishing macroscopic mean field. Transition to coherence in a chain of locally coupled oscillators described with phase equations is investigated with respect to the symmetries in the system. It is shown that the reversibility of the system caused by these symmetries results to non-trivial topological properties of trajectories so that the system constructed to be dissipative reveals in a whole parameter range quasi-Hamiltonian features, i.e. the phase volume is conserved on average and Lyapunov exponents come in symmetric pairs. Transition to coherence in an ensemble of globally coupled chaotic maps is described with the loss of stability of the disordered state. The method is to break the self-consistensy of the macroscopic field and to characterize the ensemble in analogy to an amplifier circuit with feedback with a complex linear transfer function. This theory is then generalized for several cases of theoretic interest.
Synchronization regimes in an ensemble of phase oscillators coupled through a diffusion field
(2022)
We consider an ensemble of identical phase oscillators coupled through a common diffusion field. Using the Ott-Antonsen reduction, we develop dynamical equations for the complex local order parameter and the mean field. The regions of the existence and stability are determined for the totally synchronous, partially synchronous, and asynchronous spatially homogeneous states. A procedure of searching for inhomogeneous states as periodic trajectories of an auxiliary system of the ordinary differential equations is demonstrated. A scenario of emergence of chimera structures from homogeneous synchronous solutions is described.
We present experimental and numerical evidence of synchronization of burst events in two different modulated CO2 lasers. Bursts appear randomly in each laser as trains of large amplitude spikes intercalated by a small amplitude chaotic regime. Experimental data and model show the frequency locking of bursts in a suitable interval of coupling strength. We explain the mechanism of this phenomenon and demonstrate the inhibitory properties of the implemented coupling.
Synchronization of large ensembles of oscillators is an omnipresent phenomenon observed in different fields of science like physics, engineering, life sciences, etc. The most simple setup is that of globally coupled phase oscillators, where all the oscillators contribute to a global field which acts on all oscillators. This formulation of the problem was pioneered by Winfree and Kuramoto. Such a setup gives a possibility for the analysis of these systems in terms of global variables. In this work we describe nontrivial collective dynamics in oscillator populations coupled via mean fields in terms of global variables. We consider problems which cannot be directly reduced to standard Kuramoto and Winfree models.
In the first part of the thesis we adopt a method introduced by Watanabe and Strogatz. The main idea is that the system of identical oscillators of particular type can be described by a low-dimensional system of global equations. This approach enables us to perform a complete analytical analysis for a special but vast set of initial conditions. Furthermore, we show how the approach can be expanded for some nonidentical systems. We apply the Watanabe-Strogatz approach to arrays of Josephson junctions and systems of identical phase oscillators with leader-type coupling.
In the next parts of the thesis we consider the self-consistent mean-field theory method that can be applied to general nonidentical globally coupled systems of oscillators both with or without noise. For considered systems a regime, where the global field rotates uniformly, is the most important one. With the help of this approach such solutions of the self-consistency equation for an arbitrary distribution of frequencies and coupling parameters can be found analytically in the parametric form, both for noise-free and noisy cases.
We apply this method to deterministic Kuramoto-type model with generic coupling and an ensemble of spatially distributed oscillators with leader-type coupling. Furthermore, with the proposed self-consistent approach we fully characterize rotating wave solutions of noisy Kuramoto-type model with generic coupling and an ensemble of noisy oscillators with bi-harmonic coupling.
Whenever possible, a complete analysis of global dynamics is performed and compared with direct numerical simulations of large populations.
Topic and aim. Synchronization in populations of coupled oscillators can be characterized with order parameters that describe collective order in ensembles. A dependence of the order parameter on the coupling constants is well-known for coupled periodic oscillators. The goal of the study is to extend this analysis to ensembles of oscillators with chaotic phases, moreover with phases possessing hyperbolic chaos. Models and methods. Two models are studied in the paper. One is an abstract discrete-time map, composed with a hyperbolic Bernoulli transformation and with Kuramoto dynamics. Another model is a system of coupled continuous-time chaotic oscillators, where each individual oscillator has a hyperbolic attractor of Smale-Williams type. Results. The discrete-time model is studied with the Ott-Antonsen ansatz, which is shown to be invariant under the application of the Bernoulli map. The analysis of the resulting map for the order parameter shows, that the asynchronouis state is always stable, but the synchronous one becomes stable above a certain coupling strength. Numerical analysis of the continuous-time model reveals a complex sequence of transitions from an asynchronous state to a completely synchronous hyperbolic chaos, with intermediate stages that include regimes with periodic in time mean field, as well as with weakly and strongly irregular mean field variations. Discussion. Results demonstrate that synchronization of systems with hyperbolic chaos of phases is possible, although a rather strong coupling is required. The approach can be applied to other systems of interacting units with hyperbolic chaotic dynamics.
We investigate synchronization of coupled organ pipes. Synchronization and reflection in the organ lead to undesired weakening of the sound in special cases. Recent experiments have shown that sound interaction is highly complex and nonlinear, however, we show that two delay-coupled Van-der-Pol oscillators appear to be a good model for the occurring dynamical phenomena. Here the coupling is realized as distance-dependent, or time-delayed, equivalently. Analytically, we investigate the synchronization frequency and bifurcation scenarios which occur at the boundaries of the Arnold tongues. We successfully compare our results to experimental data.
This thesis analyses synchronization phenomena occurring in large ensembles of interacting oscillatory units. In particular, the effects of nonisochronicity (frequency dependence on the oscillator's amplitude) on the macroscopic transition to synchronization are studied in detail. The new phenomena found (Anomalous Synchronization) are investigated in populations of oscillators as well as between oscillator's ensembles.
In the present work synchronization phenomena in complex dynamical systems exhibiting multiple time scales have been analyzed. Multiple time scales can be active in different manners. Three different systems have been analyzed with different methods from data analysis. The first system studied is a large heterogenous network of bursting neurons, that is a system with two predominant time scales, the fast firing of action potentials (spikes) and the burst of repetitive spikes followed by a quiescent phase. This system has been integrated numerically and analyzed with methods based on recurrence in phase space. An interesting result are the different transitions to synchrony found in the two distinct time scales. Moreover, an anomalous synchronization effect can be observed in the fast time scale, i.e. there is range of the coupling strength where desynchronization occurs. The second system analyzed, numerically as well as experimentally, is a pair of coupled CO₂ lasers in a chaotic bursting regime. This system is interesting due to its similarity with epidemic models. We explain the bursts by different time scales generated from unstable periodic orbits embedded in the chaotic attractor and perform a synchronization analysis of these different orbits utilizing the continuous wavelet transform. We find a diverse route to synchrony of these different observed time scales. The last system studied is a small network motif of limit cycle oscillators. Precisely, we have studied a hub motif, which serves as elementary building block for scale-free networks, a type of network found in many real world applications. These hubs are of special importance for communication and information transfer in complex networks. Here, a detailed study on the mechanism of synchronization in oscillatory networks with a broad frequency distribution has been carried out. In particular, we find a remote synchronization of nodes in the network which are not directly coupled. We also explain the responsible mechanism and its limitations and constraints. Further we derive an analytic expression for it and show that information transmission in pure phase oscillators, such as the Kuramoto type, is limited. In addition to the numerical and analytic analysis an experiment consisting of electrical circuits has been designed. The obtained results confirm the former findings.
Networks of coupled dynamical systems provide a powerful way to model systems with enormously complex dynamics, such as the human brain. Control of synchronization in such networked systems has far-reaching applications in many domains, including engineering and medicine. In this paper, we formulate the synchronization control in dynamical systems as an optimization problem and present a multi-objective genetic programming-based approach to infer optimal control functions that drive the system from a synchronized to a non-synchronized state and vice versa. The genetic programming-based controller allows learning optimal control functions in an interpretable symbolic form. The effectiveness of the proposed approach is demonstrated in controlling synchronization in coupled oscillator systems linked in networks of increasing order complexity, ranging from a simple coupled oscillator system to a hierarchical network of coupled oscillators. The results show that the proposed method can learn highly effective and interpretable control functions for such systems.
This work deals with the connection between two basic phenomena in Nonlinear Dynamics: synchronization of chaotic systems and recurrences in phase space. Synchronization takes place when two or more systems adapt (synchronize) some characteristic of their respective motions, due to an interaction between the systems or to a common external forcing. The appearence of synchronized dynamics in chaotic systems is rather universal but not trivial. In some sense, the possibility that two chaotic systems synchronize is counterintuitive: chaotic systems are characterized by the sensitivity ti different initial conditions. Hence, two identical chaotic systems starting at two slightly different initial conditions evolve in a different manner, and after a certain time, they become uncorrelated. Therefore, at a first glance, it does not seem to be plausible that two chaotic systems are able to synchronize. But as we will see later, synchronization of chaotic systems has been demonstrated. On one hand it is important to investigate the conditions under which synchronization of chaotic systems occurs, and on the other hand, to develop tests for the detection of synchronization. In this work, I have concentrated on the second task for the cases of phase synchronization (PS) and generalized synchronization (GS). Several measures have been proposed so far for the detection of PS and GS. However, difficulties arise with the detection of synchronization in systems subjected to rather large amounts of noise and/or instationarities, which are common when analyzing experimental data. The new measures proposed in the course of this thesis are rather robust with respect to these effects. They hence allow to be applied to data, which have evaded synchronization analysis so far. The proposed tests for synchronization in this work are based on the fundamental property of recurrences in phase space.
We have studied the bifurcations in a three-dimensional incompressible magnetofluid with periodic boundary conditions and an external forcing of the Arnold-Beltrami-Childress (ABC) type. Bifurcation-analysis techniques have been applied to explore the qualitative behavior of solution branches. Due to the symmetry of the forcing, the equations are equivariant with respect to a group of transformations isomorphic to the octahedral group, and we have paid special attention to symmetry-breaking effects. As the Reynolds number is increased, the primary nonmagnetic steady state, the ABC flow, loses its stability to a periodic magnetic state, showing the appearance of a generic dynamo effect; the critical value of the Reynolds number for the instability of the ABC flow is decreased compared to the purely hydrodynamic case. The bifurcating magnetic branch in turn is subject to secondary, symmetry-breaking bifurcations. We have traced periodic and quasi- periodic branches until they end up in chaotic states. In particular detail we have analyzed the subgroup symmetries of the bifurcating periodic branches, which are closely related to the spatial structure of the magnetic field.
In the present work, we use symbolic regression for automated modeling of dynamical systems. Symbolic regression is a powerful and general method suitable for data-driven identification of mathematical expressions. In particular, the structure and parameters of those expressions are identified simultaneously.
We consider two main variants of symbolic regression: sparse regression-based and genetic programming-based symbolic regression. Both are applied to identification, prediction and control of dynamical systems.
We introduce a new methodology for the data-driven identification of nonlinear dynamics for systems undergoing abrupt changes. Building on a sparse regression algorithm derived earlier, the model after the change is defined as a minimum update with respect to a reference model of the system identified prior to the change. The technique is successfully exemplified on the chaotic Lorenz system and the van der Pol oscillator. Issues such as computational complexity, robustness against noise and requirements with respect to data volume are investigated.
We show how symbolic regression can be used for time series prediction. Again, issues such as robustness against noise and convergence rate are investigated us- ing the harmonic oscillator as a toy problem. In combination with embedding, we demonstrate the prediction of a propagating front in coupled FitzHugh-Nagumo oscillators. Additionally, we show how we can enhance numerical weather predictions to commercially forecast power production of green energy power plants.
We employ symbolic regression for synchronization control in coupled van der Pol oscillators. Different coupling topologies are investigated. We address issues such as plausibility and stability of the control laws found. The toolkit has been made open source and is used in turbulence control applications.
Genetic programming based symbolic regression is very versatile and can be adapted to many optimization problems. The heuristic-based algorithm allows for cost efficient optimization of complex tasks.
We emphasize the ability of symbolic regression to yield white-box models. In contrast to black-box models, such models are accessible and interpretable which allows the usage of established tool chains.
Switch It Inside-Out: "Schizophrenic" Behavior of All Thermoresponsive UCST-LCST Diblock Copolymers
(2019)
This feature article reviews our recent advancements on the synthesis, phase behavior, and micellar structures of diblock copolymers consisting of oppositely thermoresponsive blocks in aqueous environments. These copolymers combine a nonionic block, which shows lower critical solution temperature (LCST) behavior, with a zwitterionic block that exhibits an upper critical solution temperature (UCST). The transition temperature of the latter class of polymers is strongly controlled by its molar mass and by the salt concentration, in contrast to the rather invariant transition of nonionic polymers with type II LCST behavior such as poly(N-isopropylacrylamide) or poly(N-isopropyl methacrylamide). This allows for implementing the sequence of the UCST and LCST transitions of the polymers at will by adjusting either molecular or, alternatively, physical parameters. Depending on the location of the transition temperatures of both blocks, different switching scenarios are realized from micelles to inverse micelles, namely via the molecularly dissolved state, the aggregated state, or directly. In addition to studies of (semi)dilute aqueous solutions, highly concentrated systems have also been explored, namely water-swollen thin films. Concerning applications, we discuss the possible use of the diblock copolymers as "smart" nanocarriers.
The ratio of the proton ring velocity (VR) to the local Alfven speed (VA), in addition to proton ring distributions, plays a key factor in the excitation of magnetosonic waves at frequencies between the proton cyclotron frequency fcp and the lower hybrid resonance frequency fLHR in the Earth's magnetosphere. Here we investigate whether there is a statistically significant relationship between occurrences of proton rings and magnetosonic waves both outside and inside the plasmapause using particle and wave data from Van Allen Probe-A during the time period of October 2012 to December 2015. We also perform a statistical survey of the ratio of the ring energy (ER, corresponding to VR) to the Alfven energy (EA, corresponding to VA) to determine the favorable conditions under which magnetosonic waves in each of two frequency bands (fcp < f ≤ 0.5 fLHR and 0.5 fLHR < f < fLHR) can be excited. The results show that the magnetosonic waves in both frequency bands occur around the postnoon (12–18 magnetic local time, MLT) sector outside the plasmapause when ER is comparable to or lower than EA, and those in lower-frequency bands (fcp < f ≤ 0.5 fLHR) occur around the postnoon sector inside the plasmapause when ER/EA > ~9. However, there is one discrepancy between occurrences of proton rings and magnetosonic waves in low-frequency bands around the prenoon sector (6–12 MLT) outside the plasmapause, which suggests either that the waves may have propagated during active time from the postnoon sector after being excited during quiet time, or they may have locally excited in the prenoon sector during active time.
Tailoring the secondary surface morphology of electro-spun nanofibers has been highly desired, as such delicate structures equip nanofibers with distinct functions. Here, we report a simple strategy to directly reconstruct the surface of polyvinyl alcohol/polyvinylpyrrolidone (PVA/PVP) nanofibers by water evaporation. The roughness and diameter of the nanofibers depend on the temperature during vacuum drying. Surface changes of the nanofibers from smooth to rough were observed at 55 degrees C, with a significant drop in nanofiber diameter. We attribute the formation of the secondary surface morphology to the intermolecular forces in the water vapor, including capillary and the compression forces, on the basis of the results from the Fourier-transform infrared (FTIR) and X-ray photoelectron (XPS) spectroscopy. The strategy is universally effective for various electro-spun polymer nanofibers, thus opening up avenues toward more detailed and sophisticated structure design and implementation for nanofibers.
This paper presents a study of the surface properties of two Ce/Zr mixed oxides with different reducibility, obtained by applying distinct thermal ageing treatments to an oxide with the composition Ce0.62Zr0.38O2. The surface composition was investigated by XPS. Chemical reactivity of the surface was studied by adsorption of the probe molecules CO2, D-2 and methanol. Nanostructural characterization was carried out by XRD, Raman and high-resolution Eu3+ spectroscopy (FLNS). The characterization showed only slight variations in surface composition and bulk Ce-Zr distribution, but hardy differences concerning the type and strength of acidic surface centres, as well as strong differences in the ability to dissociate hydrogen. Structural variations between both samples were identified by comparing the optical spectra of Eu3+ in surface doped samples.
Suppression of the TeV Pair-beam-Plasma Instability by a Tangled Weak Intergalactic Magnetic Field
(2022)
We study the effect of a tangled sub-fG level intergalactic magnetic field (IGMF) on the electrostatic instability of a blazar-induced pair beam. Sufficiently strong IGMF may significantly deflect the TeV pair beams, which would reduce the flux of secondary cascade emission below the observational limits. A similar flux reduction may result from the electrostatic beam-plasma instability, which operates the best in the absence of IGMF. Considering IGMF with correlation lengths smaller than a kiloparsec, we find that weak magnetic fields increase the transverse momentum of the pair-beam particles, which dramatically reduces the linear growth rate of the electrostatic instability and hence the energy-loss rate of the pair beam. We show that the beam-plasma instability is eliminated as an effective energy-loss agent at a field strength three orders of magnitude below that needed to suppress the secondary cascade emission by magnetic deflection. For intermediate-strength IGMF, we do not know a viable process to explain the observed absence of GeV-scale cascade emission.
We have shown that the two-dimensional complex Ginzburg-Landau equation exhibits supertransient chaos in a certain parameter range. Using numerical methods this behavior is found near the transition line separating frozen spiral solutions from turbulence. Supertransient chaos seems to be a common phenomenon in extended spatiotemporal systems. These supertransients are characterized by an average transient lifetime which depends exponentially on the size of the system and are due to an underlying nonattracting chaotic set.
Brownian motion and viscoelastic anomalous diffusion in homogeneous environments are intrinsically Gaussian processes. In a growing number of systems, however, non-Gaussian displacement distributions of these processes are being reported. The physical cause of the non-Gaussianity is typically seen in different forms of disorder. These include, for instance, imperfect "ensembles" of tracer particles, the presence of local variations of the tracer mobility in heteroegenous environments, or cases in which the speed or persistence of moving nematodes or cells are distributed. From a theoretical point of view stochastic descriptions based on distributed ("superstatistical") transport coefficients as well as time-dependent generalisations based on stochastic transport parameters with built-in finite correlation time are invoked. After a brief review of the history of Brownian motion and the famed Gaussian displacement distribution, we here provide a brief introduction to the phenomenon of non-Gaussianity and the stochastic modelling in terms of superstatistical and diffusing-diffusivity approaches.
Recent advances in single particle tracking and supercomputing techniques demonstrate the emergence of normal or anomalous, viscoelastic diffusion in conjunction with non-Gaussian distributions in soft, biological, and active matter systems. We here formulate a stochastic model based on a generalised Langevin equation in which non-Gaussian shapes of the probability density function and normal or anomalous diffusion have a common origin, namely a random parametrisation of the stochastic force. We perform a detailed analysis demonstrating how various types of parameter distributions for the memory kernel result in exponential, power law, or power-log law tails of the memory functions. The studied system is also shown to exhibit a further unusual property: the velocity has a Gaussian one point probability density but non-Gaussian joint distributions. This behaviour is reflected in the relaxation from a Gaussian to a non-Gaussian distribution observed for the position variable. We show that our theoretical results are in excellent agreement with stochastic simulations.
Recent advances in single particle tracking and supercomputing techniques demonstrate the emergence of normal or anomalous, viscoelastic diffusion in conjunction with non-Gaussian distributions in soft, biological, and active matter systems. We here formulate a stochastic model based on a generalised Langevin equation in which non-Gaussian shapes of the probability density function and normal or anomalous diffusion have a common origin, namely a random parametrisation of the stochastic force. We perform a detailed analysis demonstrating how various types of parameter distributions for the memory kernel result in exponential, power law, or power-log law tails of the memory functions. The studied system is also shown to exhibit a further unusual property: the velocity has a Gaussian one point probability density but non-Gaussian joint distributions. This behaviour is reflected in the relaxation from a Gaussian to a non-Gaussian distribution observed for the position variable. We show that our theoretical results are in excellent agreement with stochastic simulations.
Background
Due to physical coupling between mechanical stress and magnetization in ferromagnetic materials, it is assumed in the literature that the distribution of the magnetic stray field corresponds to the internal (residual) stress of the specimen.
The correlation is, however, not trivial, since the magnetic stray field is also influenced by the microstructure and the geometry of component.
The understanding of the correlation between residual stress and magnetic stray field could help to evaluate the integrity of welded components.
Objective
This study aims at understanding the possible correlation of subsurface and bulk residual stress with magnetic stray field in a low carbon steel weld.
Methods
The residual stress was determined by synchrotron X-ray diffraction (SXRD, subsurface region) and by neutron diffraction (ND, bulk region).
SXRD possesses a higher spatial resolution than ND. Magnetic stray fields were mapped by utilizing high-spatial-resolution giant magneto resistance (GMR) sensors.
Results
The subsurface residual stress overall correlates better with the magnetic stray field distribution than the bulk stress. This correlation is especially visible in the regions outside the heat affected zone, where the influence of the microstructural features is less pronounced but steep residual stress gradients are present.
Conclusions
It was demonstrated that the localized stray field sources without any obvious microstructural variations are associated with steep stress gradients.
The good correlation between subsurface residual stress and magnetic signal indicates that the source of the magnetic stray fields is to be found in the range of the penetration depth of the SXRD measurements.
Organic photovoltaics based on non-fullerene acceptors (NFAs) show record efficiency of 16 to 17% and increased photovoltage owing to the low driving force for interfacial charge-transfer. However, the low driving force potentially slows down charge generation, leading to a tradeoff between voltage and current. Here, we disentangle the intrinsic charge-transfer rates from morphology-dependent exciton diffusion for a series of polymer:NFA systems. Moreover, we establish the influence of the interfacial energetics on the electron and hole transfer rates separately. We demonstrate that charge-transfer timescales remain at a few hundred femtoseconds even at near-zero driving force, which is consistent with the rates predicted by Marcus theory in the normal region, at moderate electronic coupling and at low re-organization energy. Thus, in the design of highly efficient devices, the energy offset at the donor:acceptor interface can be minimized without jeopardizing the charge-transfer rate and without concerns about a current-voltage tradeoff.
Organic photovoltaics based on non-fullerene acceptors (NFAs) show record efficiency of 16 to 17% and increased photovoltage owing to the low driving force for interfacial charge-transfer. However, the low driving force potentially slows down charge generation, leading to a tradeoff between voltage and current. Here, we disentangle the intrinsic charge-transfer rates from morphology-dependent exciton diffusion for a series of polymer:NFA systems. Moreover, we establish the influence of the interfacial energetics on the electron and hole transfer rates separately. We demonstrate that charge-transfer timescales remain at a few hundred femtoseconds even at near-zero driving force, which is consistent with the rates predicted by Marcus theory in the normal region, at moderate electronic coupling and at low re-organization energy. Thus, in the design of highly efficient devices, the energy offset at the donor:acceptor interface can be minimized without jeopardizing the charge-transfer rate and without concerns about a current-voltage tradeoff.
Crystal structures of four different di-aryl-1,3,4-oxadiazole compounds (aryl = 2-pyridyl-, 3-pyridyl-, 2-aminophenyl-, 3-aminophenyl-) are determined. Crystallization of di(2-pyridyl)-1,3,4-oxadiazole yielded monoclinic and triclinic polymorphs. The structures are characterized by the occurrence of pi-pi interactions. Additionally, in case of the aminophenyl compounds intra- as well as intermolecular hydrogen bonds are found that influence the packing motif as well. Since these molecules are often used as ligands in metal-organic complexes similarities and differences of the molecular conformation between the molecules in the pure crystals and that of the ligands in the complexes are discussed. (c) 2006 Elsevier B.V. All rights reserved.
Poly(vinylidenefluoride-trifluoroethylene)-based (P(VDF-TrFE)-based) terpolymers represent a new class of electroactive polymer materials that are relaxor-ferroelectric (RF) polymers and that offer unique and attractive property combinations in comparison with conventional ferroelectric polymers. The RF state is achieved by introducing a fluorine-containing termonomer as a "defect" into the ferroelectric P(VDF-TrFE) copolymer, which reduces the interaction between the VDF/TrFE dipoles. The resulting terpolymer exhibits a low Curie transition temperature and small remanent and coercive fields yielding a slim hysteresis loop that is typical for RF materials. Though the macroscopic behavior is similar to RF ceramics, the mechanisms of relaxor ferroelectricity in semi-crystalline polymers are different and not fully understood yet. Structure-property relationships play an important role in RF terpolymers, as they govern the final RF properties. Hence, a review of important characteristics, previous studies and relevant developments of P(VDF-TrFE)-based terfluoropolymers with either chlorofluoroethylene (CFE) or chlorotrifluoroethylene (CTFE) as the termonomer is deemed useful. The role of the termonomer and of its composition, as well as the effects of the processing conditions on the semi-crystalline structure which in turn affects the final RF properties are discussed in detail. In addition, the presence of noteworthy transition(s) in the mid-temperature range and the influence of preparation conditions on those transitions are reviewed. A better understanding of the fundamental aspects affecting the semi-crystalline structures will help to elucidate the nature of RF activity in VDF-based terpolymers and also help to further improve their applications-relevant electroactive properties.
The mammalian brain is, with its numerous neural elements and structured complex connectivity, one of the most complex systems in nature. Recently, large-scale corticocortical connectivities, both structural and functional, have received a great deal of research attention, especially using the approach of complex networks. Here, we try to shed some light on the relationship between structural and functional connectivities by studying synchronization dynamics in a realistic anatomical network of cat cortical connectivity. We model the cortical areas by a subnetwork of interacting excitable neurons (multilevel model) and by a neural mass model (population model). With weak couplings, the multilevel model displays biologically plausible dynamics and the synchronization patterns reveal a hierarchical cluster organization in the network structure. We can identify a group of brain areas involved in multifunctional tasks by comparing the dynamical clusters to the topological communities of the network. With strong couplings of multilevel model and by using neural mass model, the dynamics are characterized by well-defined oscillations. The synchronization patterns are mainly determined by the node intensity (total input strengths of a node); the detailed network topology is of secondary importance. The biologically improved multilevel model exhibits similar dynamical patterns in the two regimes. Thus, the study of synchronization in a multilevel complex network model of cortex can provide insights into the relationship between network topology and functional organization of complex brain networks.
We present a combined microscopic and macroscopic study of YbxCo4Sb12 skutterudites for a range of nominal filling fractions, 0.15 < x < 0.75. The samples were synthesized using two different methods — a melt–quench–annealing route in evacuated quartz ampoules and a non-equilibrium ball-mill route — for which we directly compare the crystal structure and phase composition as well as the thermoelectric properties. Rietveld refinements of high-quality neutron powder diffraction data reveal about a 30–40% smaller Yb occupancy on the crystallographic 2a site than nominally expected for both synthesis routes. We observe a maximum filling fraction of at least 0.439(7) for a sample synthesized by the ball-mill routine, exceeding theoretical predictions of the filling fraction limit of 0.2–0.3. A single secondary phase of CoSb2 is observed in ball-mill-synthesized samples, while two secondary phases, CoSb2 and YbSb2, are detected for samples prepared by the ampoule route. A detrimental influence of the secondary phases on the thermoelectric properties is observed for secondary-phase fractions larger than 8 wt % regardless of the kind of secondary phase. The largest figure of merit of all samples with a ZT ∼ 1.0 at 723 K is observed for the sample with a refined Yb content of x2a = 0.159(3), synthesized by the ampoule route.
Nowadays, colloidal rods can be synthesized in large amounts. The rods are typically cylindrically and their length ranges from several nanometers to a few micrometers. In solution, systems of colloidal rodlike molecules or aggregates can form liquid-crystalline phases with long-range orientational and spatial order. In the present work, we investigate structure formation and fractionation in systems of rodlike colloids with the help of Monte Carlo simulations in the NPT ensemble. Repulsive interactions can successfully be mimicked by the hard rod model, which has been studied extensively in the past. In many cases, attractive interactions like van der Waals or depletion forces cannot be neglected, however. In the first part of this work, the phase behavior of monodisperse attractive rods is characterized for different interaction strengths. Phase diagrams as a function of rod length and pressure are presented. Most systems of synthesized mesoscopic rods have a polydisperse length distribution as a consequence of the longitudinal growth process of the rods. For many technical and research applications, a rather small polydispersity is desired in order to have well defined material properties. The polydispersity can be reduced by a spatial demixing (fractionation) of long and short rods. Fractionation and structure formation is studied in a tridisperse and a polydisperse bulk suspension of rods. We observe that the resulting structures depend distinctly on the interaction strength. The fractionation in the system is strongly enhanced with increasing interaction strength. Suspensions are typically confined in a container. We also examine the influence of adjacent substrates in systems of tridisperse and polydisperse rod suspensions. Three different substrate types are studied in detail: a planar wall, a corrugated substrate, and a substrate with rectangular cavities. We analyze the fluid structure close to the substrate and substrate controlled fractionation. The spatial arrangement of long and short rods in front of the substrate depends sensitively on the substrate structure and the pressure. Rods with a predefined length are segregated at substrates with rectangular cavities.
Structural health monitoring activities are of primal importance for managing transport infrastructure, however most SHM methodologies are based on point-based sensors that have limitations in terms of their spatial positioning requirements, cost of development and measurement range. This paper describes the progress on the SENSKIN EC project whose objective is to develop a dielectric-elastomer and micro-electronics-based sensor, formed from a large highly extensible capacitance sensing membrane supported by advanced microelectronic circuitry, for monitoring transport infrastructure bridges. Such a sensor could provide spatial measurements of strain in excess of 10%. The actual sensor along with the data acquisition module, the communication module and power electronics are all integrated into a compact unit, the SENSKIN device, which is energy-efficient, requires simple signal processing and it is easy to install over various surface types. In terms of communication, SENSKIN devices interact with each other to form the SENSKIN system; a fully distributed and autonomous wireless sensor network that is able to self-monitor. SENSKIN system utilizes Delay-/Disruption-Tolerant Networking technologies to ensure that the strain measurements will be received by the base station even under extreme conditions where normal communications are disrupted. This paper describes the architecture of the SENSKIN system and the development and testing of the first SENSKIN prototype sensor, the data acquisition system, and the communication system.
Structural dynamics of photoexcited nanolayered perovskites studied by ultrafast x-ray diffraction
(2012)
This publication-based thesis represents a contribution to the active research field of ultrafast structural dynamics in laser-excited nanostructures. The investigation of such dynamics is mandatory for the understanding of the various physical processes on microscopic scales in complex materials which have great potentials for advances in many technological applications. I theoretically and experimentally examine the coherent, incoherent and anharmonic lattice dynamics of epitaxial metal-insulator heterostructures on timescales ranging from femtoseconds up to nanoseconds. To infer information on the transient dynamics in the photoexcited crystal lattices experimental techniques using ultrashort optical and x-ray pulses are employed. The experimental setups include table-top sources as well as large-scale facilities such as synchrotron sources. At the core of my work lies the development of a linear-chain model to simulate and analyze the photoexcited atomic-scale dynamics. The calculated strain fields are then used to simulate the optical and x-ray response of the considered thin films and multilayers in order to relate the experimental signatures to particular structural processes. This way one obtains insight into the rich lattice dynamics exhibiting coherent transport of vibrational energy from local excitations via delocalized phonon modes of the samples. The complex deformations in tailored multilayers are identified to give rise to highly nonlinear x-ray diffraction responses due to transient interference effects. The understanding of such effects and the ability to precisely calculate those are exploited for the design of novel ultrafast x-ray optics. In particular, I present several Phonon Bragg Switch concepts to efficiently generate ultrashort x-ray pulses for time-resolved structural investigations. By extension of the numerical models to include incoherent phonon propagation and anharmonic lattice potentials I present a new view on the fundamental research topics of nanoscale thermal transport and anharmonic phonon-phonon interactions such as nonlinear sound propagation and phonon damping. The former issue is exemplified by the time-resolved heat conduction from thin SrRuO3 films into a SrTiO3 substrate which exhibits an unexpectedly slow heat conductivity. Furthermore, I discuss various experiments which can be well reproduced by the versatile numerical models and thus evidence strong lattice anharmonicities in the perovskite oxide SrTiO3. The thesis also presents several advances of experimental techniques such as time-resolved phonon spectroscopy with optical and x-ray photons as well as concepts for the implementation of x-ray diffraction setups at standard synchrotron beamlines with largely improved time-resolution for investigations of ultrafast structural processes. This work forms the basis for ongoing research topics in complex oxide materials including electronic correlations and phase transitions related to the elastic, magnetic and polarization degrees of freedom.
The interaction between surfaces displaying end-grafted hydrophilic polymer brushes plays important roles in biology and in many wet-technological applications. The outer surfaces of Gram-negative bacteria, for example, are composed of lipopolysaccharide (LPS) molecules exposing oligo- and polysaccharides to the aqueous environment. This unique, structurally complex biological interface is of great scientific interest as it mediates the interaction of bacteria with neighboring bacteria in colonies and biofilms. The interaction between polymer-decorated surfaces is generally coupled to the distance-dependent conformation of the polymer chains. Therefore, structural insight into the interacting surfaces is a prerequisite to understand the interaction characteristics as well as the underlying physical mechanisms. This problem has been addressed by theory, but accurate experimental data on polymer conformations under confinement are rare, because obtaining perturbation-free structural insight into buried soft interfaces is inherently difficult.
In this thesis, lipid membrane surfaces decorated with hydrophilic polymers of technological and biological relevance are investigated under controlled interaction conditions, i.e., at defined surface separations. For this purpose, dedicated sample architectures and experimental tools are developed. Via ellipsometry and neutron reflectometry pressure-distance curves and distance-dependent polymer conformations in terms of brush compression and reciprocative interpenetration are determined. Additional element-specific structural insight into the end-point distribution of interacting brushes is obtained by standing-wave x-ray fluorescence (SWXF).
The methodology is first established for poly[ethylene glycol] (PEG) brushes of defined length and grafting density. For this system, neutron reflectometry revealed pronounced brush interpenetration, which is not captured in common brush theories and therefore motivates rigorous simulation-based treatments. In the second step the same approach is applied to realistic mimics of the outer surfaces of Gram-negative bacteria: monolayers of wild type LPSs extracted from E. Coli O55:B5 displaying strain-specific O-side chains. The neutron reflectometry experiments yield unprecedented structural insight into bacterial interactions, which are of great relevance for the properties of biofilms.
Structural and spectroscopical study of crystals of 1,3,4-oxadiazole derivatives at high pressure
(2002)
In recent years the search for new materials of technological interest has given new impulses to the study of organic compounds. Organic substances possess a great number of advantages such as the possibility to adjust their properties for a given purpose by different chemical and physical techniques in the preparation process. Oxadiazole derivatives are interesting due to their use as material for light emitting diodes (LED) as well as scintillators. The physical properties of a solid depend on its structure. Different structures induce different intra- and intermolecular interactions. An advantageous method to modify the intra- as well as the intermolecular interactions of a given substance is the application of high pressure. Furthermore, using this method the chemical features of the compound are not influenced. We have investigated the influence of high pressure and high temperature on the super-molecular structure of several oxadiazole derivatives in crystalline state. From the results of this investigation an equation of state for these crystals was determined. Furthermore, the spectroscopical features of these materials under high pressure were characterized.
Recent research using the complex network approach has revealed a rich and complicated network topology in the cortical connectivity of mammalian brains. It is of importance to understand the implications of such complex network structures in the functional organization of the brain activities. Here we study this problem from the viewpoint of dynamical complex networks. We investigate synchronization dynamics on the corticocortical network of the cat by modeling each node (cortical area) of the network with a sub-network of interacting excitable neurons. We find that the network displays clustered synchronization behavior, and the dynamical clusters coincide with the topological community structures observed in the anatomical network. Our results provide insights into the relationship between the global organization and the functional specialization of the brain cortex.
The determination of the spin state of iron-bearing compounds at high pressure and temperature is crucial for our understanding of chemical and physical properties of the deep Earth. Studies on the relationship between the coordination of iron and its electronic spin structure in iron-bearing oxides, silicates, carbonates, iron alloys, and other minerals found in the Earth's mantle and core are scarce because of the technical challenges to simultaneously probe the sample at high pressures and temperatures. We used the unique properties of a pulsed and highly brilliant x-ray free electron laser (XFEL) beam at the High Energy Density (HED) instrument of the European XFEL to x-ray heat and probe samples contained in a diamond anvil cell. We heated and probed with the same x-ray pulse train and simultaneously measured x-ray emission and x-ray diffraction of an FeCO3 sample at a pressure of 51 GPa with up to melting temperatures. We collected spin state sensitive Fe K beta(1,3) fluorescence spectra and detected the sample's structural changes via diffraction, observing the inverse volume collapse across the spin transition. During x-ray heating, the carbonate transforms into orthorhombic Fe4C3O12 and iron oxides. Incipient melting was also observed. This approach to collect information about the electronic state and structural changes from samples contained in a diamond anvil cell at melting temperatures and above will considerably improve our understanding of the structure and dynamics of planetary and exoplanetary interiors.
Understanding of wave environments is critical for the understanding of how particles are accelerated and lost in space. This study shows that in the vicinity of Europa and Ganymede, that respectively have induced and internal magnetic fields, chorus wave power is significantly increased. The observed enhancements are persistent and exceed median values of wave activity by up to 6 orders of magnitude for Ganymede. Produced waves may have a pronounced effect on the acceleration and loss of particles in the Jovian magnetosphere and other astrophysical objects. The generated waves are capable of significantly modifying the energetic particle environment, accelerating particles to very high energies, or producing depletions in phase space density. Observations of Jupiter’s magnetosphere provide a unique opportunity to observe how objects with an internal magnetic field can interact with particles trapped in magnetic fields of larger scale objects.
Strong light-matter coupling can re-arrange the exciton energies in organic semiconductors. Here, we exploit strong coupling by embedding a fullerene-free organic solar cell (OSC) photo-active layer into an optical microcavity, leading to the formation of polariton peaks and a red-shift of the optical gap. At the same time, the open-circuit voltage of the device remains unaffected. This leads to reduced photon energy losses for the low-energy polaritons and a steepening of the absorption edge. While strong coupling reduces the optical gap, the energy of the charge-transfer state is not affected for large driving force donor-acceptor systems. Interestingly, this implies that strong coupling can be exploited in OSCs to reduce the driving force for electron transfer, without chemical or microstructural modifications of the photoactive layer. Our work demonstrates that the processes determining voltage losses in OSCs can now be tuned, and reduced to unprecedented values, simply by manipulating the device architecture.
In order to investigate their microcracking behaviour, the microstructures of several beta-eucryptite ceramics, obtained from glass precursor and cerammed to yield different grain sizes and microcrack densities, were characterized by laboratory and synchrotron x-ray refraction and tomography. Results were compared with those obtained from scanning electron microscopy (SEM). In SEM images, the characterized materials appeared fully dense but computed tomography showed the presence of pore clusters. Uniaxial tensile testing was performed on specimens while strain maps were recorded and analyzed by Digital Image Correlation (DIC). X-ray refraction techniques were applied on specimens before and after tensile testing to measure the amount of the internal specific surface (i.e., area per unit volume). X-ray refraction revealed that (a) the small grain size (SGS) material contained a large specific surface, originating from the grain boundaries and the interfaces of TiO2 precipitates; (b) the medium (MGS) and large grain size (LGS) materials possessed higher amounts of specific surface compared to SGS material due to microcracks, which decreased after tensile loading; (c) the precursor glass had negligible internal surface. The unexpected decrease in the internal surface of MGS and LGS after tensile testing is explained by the presence of compressive regions in the DIC strain maps and further by theoretical arguments. It is suggested that while some microcracks merge via propagation, more close mechanically, thereby explaining the observed X-ray refraction results. The mechanisms proposed would allow the development of a strain hardening route in ceramics.
The present work is part of a collaborative H2020 European funded research project called SENSKIN, that aims to improve Structural Health Monitoring (SHM) for transport infrastructure through the development of an innovative monitoring and management system for bridges based on a novel, inexpensive, skin-like sensor. The integrated SENSKIN technology will be implemented in the case of steel and concrete bridges, and tested, field-evaluated and benchmarked on actual bridge environment against a conventional health monitoring solution developed by Mistras Group Hellas. The main objective of the present work is to implement the autonomous, fully functional strain monitoring system based on commercially available off-the-shelf components, that will be used to accomplish direct comparison between the performance of the innovative SENSKIN sensors and the conventional strain sensors commonly used for structural monitoring of bridges. For this purpose, the mini Structural Monitoring System (mini SMS) of Physical Acoustics Corporation, a comprehensive data acquisition unit designed specifically for long-term unattended operation in outdoor environments, was selected. For the completion of the conventional system, appropriate foil-type strain sensors were selected, driven by special conditioners manufactured by Mistras Group. A comprehensive description of the strain monitoring system and its peripheral components is provided in this paper. For the evaluation of the integrated system’s performance and the effect of various parameters on the long-term behavior of sensors, several test steel pieces instrumented with different strain sensors configurations were prepared and tested in both laboratory and field ambient conditions. Furthermore, loading tests were performed aiming to validate the response of the system in monitoring the strains developed in steel beam elements subject to bending regimes. Representative results obtained from the above experimental tests have been included in this paper as well.
Die Arbeit stellt neu entwickelte Röntgenbeugungsmethoden vor, mit deren Hilfe der Verzerrungszustand des Kristallgitters von Halbleiter-Wafern und -Bauteilen im Detail charakterisiert werden kann. Hierzu werden die aussergewöhnlichen Eigenschaften der an modernen Synchrotrons wie der ESRF (Grenoble) verfügbaren Röntgenstrahlung genutzt. Im ersten Teil der Arbeit werden Röntgen-Diffraktometrie und -Topographie zu einer Untersuchungsmethode kombiniert, mit der die makroskopische Krümmung von Halbleiter-Wafern ebenso wie ihre mikroskopische Defektstruktur abgebildet werden kann. Der zweite Teil ist der Untersuchung von epitaktisch gewachsenen und geätzten Oberflächengittern mit Abmessungen im Submikrometer-Bereich gewidmet. Die unterschiedlichen Gitterkonstanten der beteiligten Halbleitermaterialien führen zu einem inhomogenen Verzerrungsfeld in der Probe, das sich im Röntgenbild durch eine charakteristische Verformung des Beugungsmusters in der Umgebung der Bragg-Reflexe äussert. Die Analyse der experimentell gemessenen Beugungsmuster geschieht mit Hilfe eines neu entwickelten Simulationsverfahrens, das Elastizitätstheorie und eine semi-kinematische Röntgenbeugungstheorie miteinander verbindet. Durch quantitativen Vergleich der Simulationsergebnisse mit den Messdaten kann auf den genauen Verlauf des Verzerrungsfeldes in den Proben zurückgeschlossen werden. Dieses Verfahren wird erfolgreich auf verschiedene Halbleiter-Probensysteme angewendet, und schliesslich auch auf die Untersuchung von akustischen Oberflächenwellen in Halbleiterkristallen übertragen.
We present a study of the control of electric field induced strain on the magnetic and electrical transport properties in a magnetoelastically coupled artificial multiferroic Fe3O4/BaTiO3 heterostructure.
In this Fe3O4/BaTiO3 heterostructure, the Fe3O4 thin film is epitaxially grown in the form of bilateral domains, analogous to a-c stripe domains of the underlying BaTiO3(001) substrate.
By in situ electric field dependent magnetization measurements, we demonstrate the extrinsic control of the magnetic anisotropy and the characteristic Verwey metal-insulator transition of the epitaxial Fe3O4 thin film in a wide temperature range between 20-300 K, via strain mediated converse magnetoelectric coupling.
In addition, we observe strain induced modulations in the magnetic and electrical transport properties of the Fe3O4 thin film across the thermally driven intrinsic ferroelectric and structural phase transitions of the BaTiO3 substrate.
In situ electric field dependent Raman measurements reveal that the electric field does not significantly modify the antiphase boundary defects in the Fe3O4 thin film once it is thermodynamically stable after deposition and that the modification of the magnetic properties is mainly caused by strain induced lattice distortions and magnetic anisotropy.
These results provide a framework to realize electrical control of the magnetization in a classical highly correlated transition metal oxide.
Das Manuskript dient der Vorbereitung der Prüfung der Fachkunde zum Strahlenschutz für Lehrer. Es enthält wichtige Grundlagen der Kernphysik, insbesondere die Eigenschaften der Alpha-, Beta-, Gamma-, Neutronen- und Röntgenstrahlen. Es folgt eine kurze Beschreibung des Einflusses der Strahlung auf belebte Materie. Wichtige Paragrafen der Strahlenschutzverordnung werden beschrieben. Eine Aufgabensammlung dient zur Illustration und Übung.
Accurately predicting total electron content (TEC) during geomagnetic storms is still a challenging task for ionospheric models. In this work, a neural-network (NN)-based model is proposed which predicts relative TEC with respect to the preceding 27-day median TEC, during storm time for the European region (with longitudes 30 degrees W-50 degrees E and latitudes 32.5 degrees N-70 degrees N). The 27-day median TEC (referred to as median TEC), latitude, longitude, universal time, storm time, solar radio flux index F10.7, global storm index SYM-H and geomagnetic activity index Hp30 are used as inputs and the output of the network is the relative TEC. The relative TEC can be converted to the actual TEC knowing the median TEC. The median TEC is calculated at each grid point over the European region considering data from the last 27 days before the storm using global ionosphere maps (GIMs) from international GNSS service (IGS) sources. A storm event is defined when the storm time disturbance index Dst drops below 50 nanotesla. The model was trained with storm-time relative TEC data from the time period of 1998 until 2019 (2015 is excluded) and contains 365 storms. Unseen storm data from 33 storm events during 2015 and 2020 were used to test the model. The UQRG GIMs were used because of their high temporal resolution (15 min) compared to other products from different analysis centers. The NN-based model predictions show the seasonal behavior of the storms including positive and negative storm phases during winter and summer, respectively, and show a mixture of both phases during equinoxes. The model's performance was also compared with the Neustrelitz TEC model (NTCM) and the NN-based quiet-time TEC model, both developed at the German Aerospace Agency (DLR). The storm model has a root mean squared error (RMSE) of 3.38 TEC units (TECU), which is an improvement by 1.87 TECU compared to the NTCM, where an RMSE of 5.25 TECU was found. This improvement corresponds to a performance increase by 35.6%. The storm-time model outperforms the quiet-time model by 1.34 TECU, which corresponds to a performance increase by 28.4% from 4.72 to 3.38 TECU. The quiet-time model was trained with Carrington averaged TEC and, therefore, is ideal to be used as an input instead of the GIM derived 27-day median. We found an improvement by 0.8 TECU which corresponds to a performance increase by 17% from 4.72 to 3.92 TECU for the storm-time model using the quiet-time-model predicted TEC as an input compared to solely using the quiet-time model.
Storm Time Depletions of Multi-MeV Radiation Belt Electrons Observed at Different Pitch Angles
(2019)
During geomagnetic storms, the rapid depletion of the high-energy (several MeV) outer radiation belt electrons is the result of loss to the interplanetary medium through the magnetopause, outward radial diffusion, and loss to the atmosphere due to wave-particle interactions. We have performed a statistical study of 110 storms using pitch angle resolved electron flux measurements from the Van Allen Probes mission and found that inside of the radiation belt (L* = 3 - 5) the number of storms that result in depletion of electrons with equatorial pitch angle alpha(eq) = 30 degrees is higher than number of storms that result in depletion of electrons with equatorial pitch angle alpha(eq) = 75 degrees. We conclude that this result is consistent with electron scattering by whistler and electromagnetic ion cyclotron waves. At the outer edge of the radiation belt (L* >= 5.2) the number of storms that result in depletion is also large (similar to 40-50%), emphasizing the significance of the magnetopause shadowing effect and outward radial transport.
Stochastic Wilson
(2015)
We consider a simple Markovian class of the stochastic Wilson–Cowan type models of neuronal network dynamics, which incorporates stochastic delay caused by the existence of a refractory period of neurons. From the point of view of the dynamics of the individual elements, we are dealing with a network of non-Markovian stochastic two-state oscillators with memory, which are coupled globally in a mean-field fashion. This interrelation of a higher-dimensional Markovian and lower-dimensional non-Markovian dynamics is discussed in its relevance to the general problem of the network dynamics of complex elements possessing memory. The simplest model of this class is provided by a three-state Markovian neuron with one refractory state, which causes firing delay with an exponentially decaying memory within the two-state reduced model. This basic model is used to study critical avalanche dynamics (the noise sustained criticality) in a balanced feedforward network consisting of the excitatory and inhibitory neurons. Such avalanches emerge due to the network size dependent noise (mesoscopic noise). Numerical simulations reveal an intermediate power law in the distribution of avalanche sizes with the critical exponent around −1.16. We show that this power law is robust upon a variation of the refractory time over several orders of magnitude. However, the avalanche time distribution is biexponential. It does not reflect any genuine power law dependence.
Stochastic Wilson
(2015)
We consider a simple Markovian class of the stochastic Wilson–Cowan type models of neuronal network dynamics, which incorporates stochastic delay caused by the existence of a refractory period of neurons. From the point of view of the dynamics of the individual elements, we are dealing with a network of non-Markovian stochastic two-state oscillators with memory, which are coupled globally in a mean-field fashion. This interrelation of a higher-dimensional Markovian and lower-dimensional non-Markovian dynamics is discussed in its relevance to the general problem of the network dynamics of complex elements possessing memory. The simplest model of this class is provided by a three-state Markovian neuron with one refractory state, which causes firing delay with an exponentially decaying memory within the two-state reduced model. This basic model is used to study critical avalanche dynamics (the noise sustained criticality) in a balanced feedforward network consisting of the excitatory and inhibitory neurons. Such avalanches emerge due to the network size dependent noise (mesoscopic noise). Numerical simulations reveal an intermediate power law in the distribution of avalanche sizes with the critical exponent around −1.16. We show that this power law is robust upon a variation of the refractory time over several orders of magnitude. However, the avalanche time distribution is biexponential. It does not reflect any genuine power law dependence.
Stochastic resetting, a diffusive process whose amplitude is reset to the origin at random times, is a vividly studied strategy to optimize encounter dynamics, e.g., in chemical reactions. Here we generalize the resetting step by introducing a random resetting amplitude such that the diffusing particle may be only partially reset towards the trajectory origin or even overshoot the origin in a resetting step. We introduce different scenarios for the random-amplitude stochastic resetting process and discuss the resulting dynamics. Direct applications are geophysical layering (stratigraphy) and population dynamics or financial markets, as well as generic search processes.
Stochastic information, to be understood as "information gained by the application of stochastic methods", is proposed as a tool in the assessment of changes in climate. This thesis aims at demonstrating that stochastic information can improve the consideration and reduction of uncertainty in the assessment of changes in climate. The thesis consists of three parts. In part one, an indicator is developed that allows the determination of the proximity to a critical threshold. In part two, the tolerable windows approach (TWA) is extended to a probabilistic TWA. In part three, an integrated assessment of changes in flooding probability due to climate change is conducted within the TWA. The thermohaline circulation (THC) is a circulation system in the North Atlantic, where the circulation may break down in a saddle-node bifurcation under the influence of climate change. Due to uncertainty in ocean models, it is currently very difficult to determine the distance of the THC to the bifurcation point. We propose a new indicator to determine the system's proximity to the bifurcation point by considering the THC as a stochastic system and using the information contained in the fluctuations of the circulation around the mean state. As the system is moved closer to the bifurcation point, the power spectrum of the overturning becomes "redder", i.e. more energy is contained in the low frequencies. Since the spectral changes are a generic property of the saddle-node bifurcation, the method is not limited to the THC, but it could also be applicable to other systems, e.g. transitions in ecosystems. In part two, a probabilistic extension to the tolerable windows approach (TWA) is developed. In the TWA, the aim is to determine the complete set of emission strategies that are compatible with so-called guardrails. Guardrails are limits to impacts of climate change or to climate change itself. Therefore, the TWA determines the "maneuvering space" humanity has, if certain impacts of climate change are to be avoided. Due to uncertainty it is not possible to definitely exclude the impacts of climate change considered, but there will always be a certain probability of violating a guardrail. Therefore the TWA is extended to a probabilistic TWA that is able to consider "probabilistic uncertainty", i.e. uncertainty that can be expressed as a probability distribution or uncertainty that arises through natural variability. As a first application, temperature guardrails are imposed, and the dependence of emission reduction strategies on probability distributions for climate sensitivities is investigated. The analysis suggests that it will be difficult to observe a temperature guardrail of 2°C with high probabilities of actually meeting the target. In part three, an integrated assessment of changes in flooding probability due to climate change is conducted. A simple hydrological model is presented, as well as a downscaling scheme that allows the reconstruction of the spatio-temporal natural variability of temperature and precipitation. These are used to determine a probabilistic climate impact response function (CIRF), a function that allows the assessment of changes in probability of certain flood events under conditions of a changed climate. The assessment of changes in flooding probability is conducted in 83 major river basins. Not all floods can be considered: Events that either happen very fast, or affect only a very small area can not be considered, but large-scale flooding due to strong longer-lasting precipitation events can be considered. Finally, the probabilistic CIRFs obtained are used to determine emission corridors, where the guardrail is a limit to the fraction of world population that is affected by a predefined shift in probability of the 50-year flood event. This latter analysis has two main results. The uncertainty about regional changes in climate is still very high, and even small amounts of further climate change may lead to large changes in flooding probability in some river systems.
We introduce and study a Lévy walk (LW) model of particle spreading with a finite propagation speed combined with soft resets, stochastically occurring periods in which an harmonic external potential is switched on and forces the particle towards a specific position. Soft resets avoid instantaneous relocation of particles that in certain physical settings may be considered unphysical. Moreover, soft resets do not have a specific resetting point but lead the particle towards a resetting point by a restoring Hookean force. Depending on the exact choice for the LW waiting time density and the probability density of the periods when the harmonic potential is switched on, we demonstrate a rich emerging response behaviour including ballistic motion and superdiffusion. When the confinement periods of the soft-reset events are dominant, we observe a particle localisation with an associated non-equilibrium steady state. In this case the stationary particle probability density function turns out to acquire multimodal states. Our derivations are based on Markov chain ideas and LWs with multiple internal states, an approach that may be useful and flexible for the investigation of other generalised random walks with soft and hard resets. The spreading efficiency of soft-rest LWs is characterised by the first-passage time statistic.
We introduce and study a Lévy walk (LW) model of particle spreading with a finite propagation speed combined with soft resets, stochastically occurring periods in which an harmonic external potential is switched on and forces the particle towards a specific position. Soft resets avoid instantaneous relocation of particles that in certain physical settings may be considered unphysical. Moreover, soft resets do not have a specific resetting point but lead the particle towards a resetting point by a restoring Hookean force. Depending on the exact choice for the LW waiting time density and the probability density of the periods when the harmonic potential is switched on, we demonstrate a rich emerging response behaviour including ballistic motion and superdiffusion. When the confinement periods of the soft-reset events are dominant, we observe a particle localisation with an associated non-equilibrium steady state. In this case the stationary particle probability density function turns out to acquire multimodal states. Our derivations are based on Markov chain ideas and LWs with multiple internal states, an approach that may be useful and flexible for the investigation of other generalised random walks with soft and hard resets. The spreading efficiency of soft-rest LWs is characterised by the first-passage time statistic.
In this thesis the interplay between hydrodynamic transport and specific adhesion is theoretically investigated. An important biological motivation for this work is the rolling adhesion of white blood cells experimentally investigated in flow chambers. There, specific adhesion is mediated by weak bonds between complementary molecular building blocks which are either located on the cell surface (receptors) or attached to the bottom plate of the flow chamber (ligands). The model system under consideration is a hard sphere covered with receptors moving above a planar ligand-bearing wall. The motion of the sphere is influenced by a simple shear flow, deterministic forces, and Brownian motion. An algorithm is given that allows to numerically simulate this motion as well as the formation and rupture of bonds between receptors and ligands. The presented algorithm spatially resolves receptors and ligands. This opens up the perspective to apply the results also to flow chamber experiments done with patterned substrates based on modern nanotechnological developments. In the first part the influence of flow rate, as well as of the number and geometry of receptors and ligands, on the probability for initial binding is studied. This is done by determining the mean time that elapses until the first encounter between a receptor and a ligand occurs. It turns out that besides the number of receptors, especially the height by which the receptors are elevated above the surface of the sphere plays an important role. These findings are in good agreement with observations of actual biological systems like white blood cells or malaria-infected red blood cells. Then, the influence of bonds which have formed between receptors and ligands, but easily rupture in response to force, on the motion of the sphere is studied. It is demonstrated that different states of motion-for example rolling-can be distinguished. The appearance of these states depending on important model parameters is then systematically investigated. Furthermore, it is shown by which bond property the ability of cells to stably roll in a large range of applied flow rates is increased. Finally, the model is applied to another biological process, the transport of spherical cargo particles by molecular motors. In analogy to the so far described systems molecular motors can be considered as bonds that are able to actively move. In this part of the thesis the mean distance the cargo particles are transported is determined.
Adhesion of biological cells to their environment is mediated by two-dimensional clusters of specific adhesion molecules which are assembled in the plasma membrane of the cells. Due to the activity of the cells or external influences, these adhesion sites are usually subject to physical forces. In recent years, the influence of such forces on the stability of cellular adhesion clusters was increasingly investigated. In particular, experimental methods that were originally designed for the investigation of single bond rupture under force have been applied to investigate the rupture of adhesion clusters. The transition from single to multiple bonds, however, is not trivial and requires theoretical modelling. Rupture of biological adhesion molecules is a thermally activated, stochastic process. In this work, a stochastic model for the rupture and rebinding dynamics of clusters of parallel adhesion molecules under force is presented. In particular, the influence of (i) a constant force as it may be assumed for cellular adhesion clusters is investigated and (ii) the influence of a linearly increasing force as commonly used in experiments is considered. Special attention is paid to the force-mediated cooperativity of parallel adhesion bonds. Finally, the influence of a finite distance between receptors and ligands on the binding dynamics is investigated. Thereby, the distance can be bridged by polymeric linker molecules which tether the ligands to a substrate.
We develop a model of stochastic radiation pressure for rotating non-spherical particles and apply the model to circumplanetary dynamics of dust grains. The stochastic properties of the radiation pressure are related to the ensemble-averaged characteristics of the rotating particles, which are given in terms of the rotational time-correlation function of a grain. We investigate the model analytically and show that an ensemble of particle trajectories demonstrates a diffusion-like behaviour. The analytical results are compared with numerical simulations, performed for the motion of the dusty ejecta from Deimos in orbit around Mars. We find that the theoretical predictions are in a good agreement with the simulation results. The agreement however deteriorates at later time, when the impact of non-linear terms, neglected in the analytic approach, becomes significant. Our results indicate that the stochastic modulation of the radiation pressure can play an important role in the circumplanetary dynamics of dust and may in case of some dusty systems noticeably alter an optical depth. (c) 2006 Elsevier Ltd. All rights reserved.
We show that "stochastic bursting" is observed in a ring of unidirectional delay-coupled noisy excitable systems, thanks to the combinational action of time-delayed coupling and noise. Under the approximation of timescale separation, i.e., when the time delays in each connection are much larger than the characteristic duration of the spikes, the observed rather coherent spike pattern can be described by an idealized coupled point processwith a leader-follower relationship. We derive analytically the statistics of the spikes in each unit, the pairwise correlations between any two units, and the spectrum of the total output from the network. Theory is in good agreement with the simulations with a network of theta-neurons. Published under license by AIP Publishing.
With the implementation of intense, short pulsed light sources throughout the last years, the powerful technique of resonant inelastic X-ray scattering (RIXS) became feasible for a wide range of experiments within femtosecond dynamics in correlated materials and molecules.
In this thesis I investigate the potential to bring RIXS into the fluence regime of nonlinear X-ray-matter interactions, especially focusing on the impact of stimulated scattering on RIXS in transition metal systems in a transmission spectroscopy geometry around transition metal L-edges.
After presenting the RIXS toolbox and the capabilities of free electron laser light sources for ultrafast intense X-ray experiments, the thesis explores an experiment designed to understand the impact of stimulated scattering on diffraction and direct beam transmission spectroscopy on a CoPd multilayer system. The experiments require short X-ray pulses that can only be generated at free electron lasers (FEL). Here the pulses are not only short, but also very intense, which opens the door to nonlinear X-ray-matter interactions. In the second part of this thesis, we investigate observations in the nonlinear interaction regime, look at potential difficulties for classic spectroscopy and investigate possibilities to enhance the RIXS through stimulated scattering. Here, a study on stimulated RIXS is presented, where we investigate the light field intensity dependent CoPd demagnetization in transmission as well as scattering geometry. Thereby we show the first direct observation of stimulated RIXS as well as light field induced nonlinear effects,
namely the breakdown of scattering intensity and the increase in sample transmittance. The topic is of ongoing interest and will just increase in relevance as more free electron lasers are planned and the number of experiments at such light sources will continue to increase in the near future.
Finally we present a discussion on the accessibility of small DOS shifts in the absorption-band of transition metal complexes through stimulated resonant X-ray scattering. As these shifts occur for example in surface states this finding could expand the experimental selectivity of NEXAFS and RIXS to the detectability of surface states. We show how stimulation can indeed enhance the visibility of DOS shifts through the detection of stimulated spectral shifts and enhancements in this theoretical study. We also forecast the observation of stimulated enhancements in resonant excitation experiments at FEL sources in systems with a high density of states just below the Fermi edge and in systems with an occupied to unoccupied DOS ratio in the valence band above 1.
We present a feasibility study with several magnetic field configurations for creating spin-dependent forces that can split a low-energy ion beam by the Stern-Gerlach (SG) effect. To the best of our knowledge, coherent spin-splittings of charged particles have yet to be realised. Our proposal is based on ion source parameters taken from a recent experiment that demonstrated single-ion implantation from a high-brightness ion source combined with a radio-frequency Paul trap. The inhomogeneous magnetic fields can be created by permanently magnetised microstructures or from current-carrying wires with sizes in the micron range, such as those recently used in a successful implementation of the SG effect with neutral atoms. All relevant forces (Lorentz force and image charges) are taken into account, and measurable splittings are found by analytical and numerical calculations.
Beim Resonanzenergietransfer werden Fotonen von einem angeregten Donator über einen Wechselwirkungsabstand auf einen Akzeptor übertragen. Nach der quantenmechanischen Theorie von FÖRSTER kann dieser Abstand mit Hilfe des Überlappungsintegrals von Fluoreszenzspektrum des Donators und Absorp-tionsspektrum des Akzeptors berechnet werden.
Eine andere Möglichkeit der Bestimmung erhält man mit Hilfe von statistischen Modellen, die in einem Überblick zusammengestellt sind. Dabei kann der Abstand durch Auswertung der Löschkurve bestimmt werden.
In dieser Arbeit wird dazu eine weitere statistische Variante der Bestimmung des Wechselwirkungsradius hinzugefügt und an einem Beispiel ausführlich demonstriert.
Beim Resonanzenergietransfer werden Fotonen von einem angeregten Donator über einen Wechselwirkungsabstand auf einen Akzeptor übertragen. Nach der quantenmechanischen Theorie von FÖRSTER kann dieser Abstand mit Hilfe des Überlappungsintegrals von Fluoreszenzspektrum des Donators und Absorp-tionsspektrum des Akzeptors berechnet werden.
Eine andere Möglichkeit der Bestimmung erhält man mit Hilfe von statistischen Modellen, die in einem Überblick zusammengestellt sind. Dabei kann der Abstand durch Auswertung der Löschkurve bestimmt werden.
In dieser Arbeit wird dazu eine weitere statistische Variante der Bestimmung des Wechselwirkungsradius hinzugefügt und an einem Beispiel ausführlich demonstriert.
Statistical properties of a free-electron laser revealed by Hanbury Brown-Twiss interferometry
(2017)
We present a comprehensive experimental analysis of statistical properties of the self-amplified spontaneous emission free-electron laser (FEL) FLASH by means of Hanbury Brown and Twiss interferometry. The experiments were performed at FEL wavelengths of 5.5, 13.4, and 20.8 nm. We determined the second-order intensity correlation function for all wavelengths and different operation conditions of FLASH. In all experiments a high degree of spatial coherence (above 50%) was obtained. Our analysis performed in spatial and spectral domains provided us with the independent measurements of an average pulse duration of the FEL that were below 60 fs. To explain the complicated behavior of the second-order intensity correlation function we developed an advanced theoretical model that includes the presence of multiple beams and external positional jitter of the FEL pulses. By this analysis we determined that in one of the experiments external positional jitter was about 25% of the beam size. We envision that methods developed in our study will be used widely for analysis and diagnostics of FEL radiation.
This work incorporates three treatises which are commonly concerned with a stochastic theory of the Lyapunov exponents. With the help of this theory universal scaling laws are investigated which appear in coupled chaotic and disordered systems. First, two continuous-time stochastic models for weakly coupled chaotic systems are introduced to study the scaling of the Lyapunov exponents with the coupling strength (coupling sensitivity of chaos). By means of the the Fokker-Planck formalism scaling relations are derived, which are confirmed by results of numerical simulations. Next, coupling sensitivity is shown to exist for coupled disordered chains, where it appears as a singular increase of the localization length. Numerical findings for coupled Anderson models are confirmed by analytic results for coupled continuous-space Schrödinger equations. The resulting scaling relation of the localization length resembles the scaling of the Lyapunov exponent of coupled chaotic systems. Finally, the statistics of the exponential growth rate of the linear oscillator with parametric noise are studied. It is shown that the distribution of the finite-time Lyapunov exponent deviates from a Gaussian one. By means of the generalized Lyapunov exponents the parameter range is determined where the non-Gaussian part of the distribution is significant and multiscaling becomes essential.
We provide a detailed stochastic description of the swimming motion of an E. coli bacterium in two dimension, where we resolve tumble events in time. For this purpose, we set up two Langevin equations for the orientation angle and speed dynamics. Calculating moments, distribution and autocorrelation functions from both Langevin equations and matching them to the same quantities determined from data recorded in experiments, we infer the swimming parameters of E. coli. They are the tumble rate lambda, the tumble time r(-1), the swimming speed v(0), the strength of speed fluctuations sigma, the relative height of speed jumps eta, the thermal value for the rotational diffusion coefficient D-0, and the enhanced rotational diffusivity during tumbling D-T. Conditioning the observables on the swimming direction relative to the gradient of a chemoattractant, we infer the chemotaxis strategies of E. coli. We confirm the classical strategy of a lower tumble rate for swimming up the gradient but also a smaller mean tumble angle (angle bias). The latter is realized by shorter tumbles as well as a slower diffusive reorientation. We also find that speed fluctuations are increased by about 30% when swimming up the gradient compared to the reversed direction.
Statistical Analysis of Hiss Waves in Plasmaspheric Plumes Using Van Allen Probe Observations
(2019)
Plasmaspheric hiss waves commonly observed in high‐density regions in the Earth's magnetosphere are known to be one of the main contributors to the loss of radiation belt electrons. There has been a lot of effort to investigate the distributions of hiss waves in the plasmasphere, while relatively little attention has been given to those in the plasmaspheric plume. In this study, we present for the first time a statistical analysis of the occurrence and the spatial distribution of wave amplitudes and wave normal angles for hiss waves in plumes using Van Allen Probes observations during the period of October 2012 to December 2016. Statistical results show that a wide range of hiss wave amplitudes in plumes from a few picotesla to >100 pT is observed, but a modest (<20 pT) wave amplitude is more commonly observed regardless of geomagnetic activity in both the midnight‐to‐dawn and dusk sector. By contrast, stronger amplitude hiss occurs preferentially during geomagnetically active times in the dusk sector. The wave normal angles are distributed over a broad range from 0° to 90° with a bimodal distribution: a quasi‐field‐aligned population (<20°) with an occurrence rate of <60% and an oblique one (>50°) with a relative low occurrence rate of ≲20%. Therefore, from a statistical point of view, we confirm that the hiss intensity (a few tens of picotesla) and field‐aligned hiss wave adopted in previous simulation studies are a reasonable assumption but stress that the activity dependence of the wave amplitude should be considered.
In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 +/- 1.0, 13.2 +/- 1.0, and 13.5 +/- 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ?+/- 0.5, 4.7 +/- 0.3, and 3.3 +/- 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices.
In the course of this thesis gold nanoparticle/polyelectrolyte multilayer structures were prepared, characterized, and investigated according to their static and ultrafast optical properties. Using the dip-coating or spin-coating layer-by-layer deposition method, gold-nanoparticle layers were embedded in a polyelectrolyte environment with high structural perfection. Typical structures exhibit four repetition units, each consisting of one gold-particle layer and ten double layers of polyelectrolyte (cationic+anionic polyelectrolyte). The structures were characterized by X-ray reflectivity measurements, which reveal Bragg peaks up to the seventh order, evidencing the high stratication of the particle layers. In the same measurements pronounced Kiessig fringes were observed, which indicate a low global roughness of the samples. Atomic force microscopy (AFM) images veried this low roughness, which results from the high smoothing capabilities of polyelectrolyte layers. This smoothing effect facilitates the fabrication of stratified nanoparticle/polyelectrolyte multilayer structures, which were nicely illustrated in a transmission electron microscopy image. The samples' optical properties were investigated by static spectroscopic measurements in the visible and UV range. The measurements revealed a frequency shift of the reflectance and of the plasmon absorption band, depending on the thickness of the polyelectrolyte layers that cover a nanoparticle layer. When the covering layer becomes thicker than the particle interaction range, the absorption spectrum becomes independent of the polymer thickness. However, the reflectance spectrum continues shifting to lower frequencies (even for large thicknesses). The range of plasmon interaction was determined to be in the order of the particle diameter for 10 nm, 20 nm, and 150 nm particles. The transient broadband complex dielectric function of a multilayer structure was determined experimentally by ultrafast pump-probe spectroscopy. This was achieved by simultaneous measurements of the changes in the reflectance and transmittance of the excited sample over a broad spectral range. The changes in the real and imaginary parts of the dielectric function were directly deduced from the measured data by using a recursive formalism based on the Fresnel equations. This method can be applied to a broad range of nanoparticle systems where experimental data on the transient dielectric response are rare. This complete experimental approach serves as a test ground for modeling the dielectric function of a nanoparticle compound structure upon laser excitation.
Amphiphilic molecules contain a hydrophilic headgroup and a hydrophobic tail. The headgroup is polar or ionic and likes water, the tail is typically an aliphatic chain that cannot be accommodated in a polar environment. The prevailing molecular asymmetry leads to a spontaneous adsorption of amphiphiles at the air/water or oil/water interfaces. As a result, the surface tension and the surface rheology is changed. Amphiphiles are important tools to deliberately modify the interfacial properties of liquid interfaces and enable new phenomena such as foams which cannot be formed in a pure liquid. In this thesis we investigate the static and dynamic properties of adsorption layers of soluble amphiphiles at the air/water interface, the so called Gibbs monolayers. The classical way for an investigation of these systems is based on a thermodynamic analysis of the equilibrium surface tension as a function of the bulk composition in the framework of Gibbs theory. However, thermodynamics does not provide any structural information and several recent publications challenge even fundamental text book concepts. The experimental investigation faces difficulties imposed by the low surface coverage and the presence of dissolved amphiphiles in the adjacent bulk phase. In this thesis we used a suite of techniques with the sensitivity to detect less than a monolayer of molecules at the air-water interface. Some of these techniques are extremely complex such as infrared visible sum frequency generation (IR-VIS SFG) spectroscopy or second harmonic generation (SHG). Others are traditional techniques, such as ellipsometry employed in new ways and pushed to new limits. Each technique probes selectively different parts of the interface and the combination provides a profound picture of the interfacial architecture. The first part of the thesis is dedicated to the distribution of ions at interfaces. Adsorption layers of ionic amphiphiles serve as model systems allowing to produce a defined surface charge. The charge of the monolayer is compensated by the counterions. As a result of a complex zoo of interactions there will be a defined distribution of ions at the interface, however, its experimental determination is a big scientific challenge. We could demonstrate that a combination of linear and nonlinear techniques gives direct insights in the prevailing ion distribution. Our investigations reveal specific ion effects which cannot be described by classical Poisson-Boltzmann mean field type theories. Adsorption layer and bulk phase are in thermodynamic equilibrium, however, it is important to stress that there is a constant molecular exchange between adsorbed and dissolved species. This exchange process is a key element for the understanding of some of the thermodynamic properties. An excellent way to study Gibbs monolayers is to follow the relaxation from a non-equilibrium to an equilibrium state. Upon compression amphiphiles must leave the adsorption layer and dissolve in the adjacent bulk phase. Upon expansion amphiphiles must adsorb at the interface to restore the equilibrium coverage. Obviously the frequency of the expansion and compression cycles must match the molecular exchange processes. At too low frequencies the equilibrium is maintained at all times. If the frequency is too fast the system behaves as a monolayer of insoluble surfactants. In this thesis we describe an unique variant of an oscillating bubble technique that measures precisely the real and imaginary part of the complex dilational modulus E in a frequency range up to 500 Hz. The extension of about two decades in the time domain in comparison to the conventional method of an oscillating drop is a tremendous achievement. The imaginary part of the complex dilational modulus E is a consequence of a dissipative process which is interpreted as an intrinsic surface dilational viscosity. The IR-VIS SFG spectra of the interfacial water provide a molecular interpretation of the underlying dissipative process.
We investigate the bias dependence of the hybrid charge transfer state emission at planar heterojunctions between the metal oxide acceptor ZnO and three donor molecules. The electroluminescence peak energy linearly increases with the applied bias, saturating at high fields. Variation of the organic layer thickness and deliberate change of the ZnO conductivity through controlled photodoping allow us to confirm that this bias-induced spectral shift relates to the internal electric field in the organic layer rather than the filling of states at the hybrid interface. We show that existing continuum models overestimate the hole delocalization and propose a simple electrostatic model in which the linear and quadratic Stark effects are explained by the electrostatic interaction of a strongly polarizable molecular cation with its mirror image.
Based on micromagnetic simulations and experimental observations of the magnetization and lattice dynamics after the direct optical excitation of the magnetic insulator Bi : YIG or indirect excitation via an optically opaque Pt/Cu double layer, we disentangle the dynamical effects of magnetic anisotropy and magneto-elastic coupling. The strain and temperature of the lattice are quantified via modeling ultrafast x-ray diffraction data. Measurements of the time-resolved magneto-optical Kerr effect agree well with the magnetization dynamics simulated according to the excitation via two mechanisms: the magneto-elastic coupling to the experimentally verified strain dynamics and the ultrafast temperature-induced transient change in the magnetic anisotropy. The numerical modeling proves that, for direct excitation, both mechanisms drive the fundamental mode with opposite phase. The relative ratio of standing spin wave amplitudes of higher-order modes indicates that both mechanisms are substantially active.
There is evidence that a self-sustaining ice discharge from the West Antarctic Ice Sheet (WAIS) has started, potentially leading to its disintegration. The associated sea level rise of more than 3m would pose a serious challenge to highly populated areas including metropolises such as Calcutta, Shanghai, New York City, and Tokyo. Here, we show that the WAIS may be stabilized through mass deposition in coastal regions around Pine Island and Thwaites glaciers. In our numerical simulations, a minimum of 7400 Gt of additional snowfall stabilizes the flow if applied over a short period of 10 years onto the region (-2 mm year(-1) sea level equivalent). Mass deposition at a lower rate increases the intervention time and the required total amount of snow. We find that the precise conditions of such an operation are crucial, and potential benefits need to be weighed against environmental hazards, future risks, and enormous technical challenges.
Owing to global warming and particularly high regional ocean warming, both Thwaites and Pine Island Glaciers in the Amundsen region of the Antarctic Ice Sheet could lose their buttressing ice shelves over time. We analyse the possible consequences using the parallel ice sheet model (PISM), applying a simple cliff-calving parameterization and an ice melange-buttressing model. We find that the instantaneous loss of ice-shelf buttressing, due to enforced ice-shelf melting, initiates grounding-line retreat and triggers marine ice sheet instability (MISI). As a consequence, the grounding line progresses into the interior of the West Antarctic Ice Sheet and leads to a sea level contribution of 0.6 m within 100 a. By subjecting the exposed ice cliffs to cliff calving using our simplified parameterization, we also analyse marine ice cliff instability (MICI). In our simulations it can double or even triple the sea level contribution depending on the only loosely constrained parameter that determines the maximum cliff-calving rate. The speed of MICI depends on this upper bound of the calving rate, which is given by the ice melange buttressing the glacier. However, stabilization of MICI may occur for geometric reasons. Because the embayment geometry changes as MICI advances into the interior of the ice sheet, the upper bound on calving rates is reduced and the progress of MICI is slowed down. Although we cannot claim that our simulations bear relevant quantitative estimates of the effect of ice-melange buttressing on MICI, the mechanism has the potential to stop the instability. Further research is needed to evaluate its role for the past and future evolution of the Antarctic Ice Sheet.
Organic thin film transistors (TFT) are an attractive option for low cost electronic applications and may be used for active matrix displays and for RFID applications. To extend the range of applications there is a need to develop and optimise the performance of non-volatile memory devices that are compatible with the solution-processing fabrication procedures used in plastic electronics. A possible candidate is an organic TFT incorporating the ferroelectric co-polymer poly(vinylidenefluoride-trifluoroethylene)(P(VDF-TrFE)) as the gate insulator. Dielectric measurements have been carried out on all-organic metal-insulator-semiconductor structures with the ferroelectric polymer poly(vinylidenefluoride-trifluoroethylene) (P(VDF-TrFE)) as the gate insu-lator. The capacitance spectra of MIS devices, were measured under different biases, showing the effect of charge accumulation and depletion on the Maxwell-Wagner peak. The position and height of this peak clearly indicates the lack of stable depletion behavior and the decrease of mobility when increasing the depletion zone width, i.e. upon moving into the P3HT bulk. The lack of stable depletion was further investigated with capacitance-voltage (C-V) measurements. When the structure was driven into depletion, C-V plots showed a positive flat-band voltage shift, arising from the change in polarization state of the ferroelectric insulator. When biased into accumulation, the polarization was reversed. It is shown that the two polarization states are stable i.e. no depolarization occurs below the coercive field. However, negative charge trapped at the semiconductor-insulator interface during the depletion cycle masks the negative shift in flat-band voltage expected during the sweep to accumulation voltages. The measured output characteristics of the studied ferroelectric-field-effect transistors confirmed the results of the C-V plots. Furthermore, the results indicated a trapping of electrons at the positively charged surfaces of the ferroelectrically polarized P(VDF-TrFE) crystallites near the insulator/semiconductor in-terface during the first poling cycles. The study of the MIS structure by means of thermally stimulated current (TSC) revealed further evidence for the stability of the polarization under depletion voltages. It was shown, that the lack of stable depletion behavior is caused by the compensation of the orientational polarization by fixed electrons at the interface and not by the depolarization of the insulator, as proposed in several publications. The above results suggest a performance improvement of non-volatile memory devices by the optimization of the interface.