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Institute
- Institut für Physik und Astronomie (150) (remove)
We implemented an experimental scheme for ultrafast x-ray diffraction at storage rings based on a laser-driven Bragg-switch that shortens the x-ray pulses emitted from an undulator. The increased time-resolution is demonstrated by observing changes of intensity, position and width of the diffraction peaks of a La(0.7)Sr(0.3)MnO(3)/SrTiO(3) superlattice sample after optical excitation, i.e., by quantitatively measuring the propagation of an expansion wave through the sample. These experimental transients with timescales of 35 to 60 ps evidence a reduction of the x-ray pulse duration by a factor of two.
Importance of polar solvation for cross-reactivity of antibody and its variants with steroids
(2011)
Understanding the factors determining the binding of ligands to receptors in detail is essential for rational drug design. Here, the free energies of binding of the steroids progesterone (PRG) and 5 beta-androstane-3,17-dione (SAD) to the Diels-Alderase antibody 1E9, as well as the Leu(H47)Trp/Arg(H100)Trp 1E9 double mutant (1E9dm) and the corresponding single mutants, have been estimated and decomposed using the molecular mechanics-Poisson-Boltzmann surface area (MM-PBSA) method. Also the difference in binding free energies between the PRG-1E9dm complex and the complex of PRG with the antiprogesterone antibody DB3 have been evaluated and decomposed. The steroids bind less strongly to 1E9 than to DB3, but the mutations tend to improve the steroid affinity, in quantitative agreement with experimental data. Although the complexes formed by PRG or SAD with 1E9dm and by PRG with DB3 have similar affinity, the binding mechanisms are different. Reduced Waals for SAD-1E9dm versus PRG-1E9dm or for PRG-1E9dm versus PRG-DB3 are energetically compensated by an increased solvation of polar groups, partly contrasting previous conclusions based on structural inspection. Our study illustrates that deducing binding mechanisms from structural models alone can be misleading. Therefore, taking into account solvation effects as in MM-PBSA calculations is essential to elucidate molecular recognition.
The discovery of a plume of water vapour and ice particles emerging from warm fractures ('tiger stripes') in Saturn's small, icy moon Enceladus(1-6) raised the question of whether the plume emerges from a subsurface liquid source(6-8) or from the decomposition of ice(9-12). Previous compositional analyses of particles injected by the plume into Saturn's diffuse E ring have already indicated the presence of liquid water(8), but the mechanisms driving the plume emission are still debated(13). Here we report an analysis of the composition of freshly ejected particles close to the sources. Salt-rich ice particles are found to dominate the total mass flux of ejected solids (more than 99 per cent) but they are depleted in the population escaping into Saturn's E ring. Ice grains containing organic compounds are found to be more abundant in dense parts of the plume. Whereas previous Cassini observations were compatible with a variety of plume formation mechanisms, these data eliminate or severely constrain non-liquid models and strongly imply that a salt-water reservoir with a large evaporating surface(7,8) provides nearly all of the matter in the plume.
To asymptotic complete scattering systems {M(+) + V, M(+)} on H(+) := L(2)(R(+), K, d lambda), where M(+) is the multiplication operator on H(+) and V is a trace class operator with analyticity conditions, a decay semigroup is associated such that the spectrum of the generator of this semigroup coincides with the set of all resonances (poles of the analytic continuation of the scattering matrix into the lower half plane across the positive half line), i.e. the decay semigroup yields a "time-dependent" characterization of the resonances. As a counterpart a "spectral characterization" is mentioned which is due to the "eigenvalue-like" properties of resonances.
Context. The Galactic gamma-ray diffuse emission is currently observed in the GeV-TeV energy range with unprecedented accuracy by the Fermi satellite. Understanding this component is crucial because it provides a background to many different signals, such as extragalactic sources or annihilating dark matter. It is timely to reinvestigate how it is calculated and to assess the various uncertainties that are likely to affect the accuracy of the predictions.
Aims. The Galactic gamma-ray diffuse emission is mostly produced above a few GeV by the interactions of cosmic ray primaries impinging on the interstellar material. The theoretical error on that component is derived by exploring various potential sources of uncertainty. Particular attention is paid to cosmic ray propagation. Nuclear cross sections, the proton and helium fluxes at the Earth's position, the Galactic radial profile of supernova remnants, and the hydrogen distribution can also severely affect the signal.
Methods. The propagation of cosmic ray species throughout the Galaxy is described in the framework of a semi-analytic two-zone diffusion/convection model. The gamma-ray flux is reliably and quickly determined. This allows conversion of the constraints set by the boron-to-carbon data into a theoretical uncertainty on the diffuse emission. New deconvolutions of the HI and CO sky maps are also used to get the hydrogen distribution within the Galaxy.
Results. The thickness of the cosmic ray diffusive halo is found to have a significant effect on the Galactic gamma-ray diffuse emission, while the interplay between diffusion and convection has little influence on the signal. The uncertainties related to nuclear cross sections and to the primary cosmic ray fluxes at the Earth are significant. The radial distribution of supernova remnants along the Galactic plane turns out to be a key ingredient. As expected, the predictions are extremely sensitive to the spatial distribution of hydrogen within the Milky Way.
Conclusions. Most of the sources of uncertainty are likely to be reduced in the near future. The stress should be put (i) on better determination of the thickness of the cosmic ray diffusive halo; and (ii) on refined observations of the radial profile of supernova remnants.
Characterization and calibration of piezoelectric polymers in situ measurements of body vibrations
(2011)
Piezoelectric polymers are known for their flexibility in applications, mainly due to their bending ability, robustness, and variable sensor geometry. It is an optimal material for minimal-invasive investigations in vibrational systems, e.g., for wood, where acoustical impedance matches particularly well. Many applications may be imagined, e. g., monitoring of buildings, vehicles, machinery, alarm systems, such that our investigations may have a large impact on technology. Longitudinal piezoelectricity converts mechanical vibrations normal to the polymer-film plane into an electrical signal, and the respective piezoelectric coefficient needs to be carefully determined in dependence on the relevant material parameters. In order to evaluate efficiency and durability for piezopolymers, we use polyvinylidene fluoride and measure the piezoelectric coefficient with respect to static pressure, amplitude of the dynamically applied force, and long-term stability. A known problem is the slow relaxation of the material towards equilibrium, if the external pressure changes; here, we demonstrate how to counter this problem with careful calibration. Since our focus is on acoustical measurements, we determine accurately the frequency response curve - for acoustics probably the most important characteristic. Eventually, we show that our piezopolymer transducers can be used as a calibrated acoustical sensors for body vibration measurements on a wooden musical instrument, where it is important to perform minimal-invasive measurements. A comparison with the simultaneously recorded airborne sound yields important insight of the mechanism of sound radiation in comparison with the sound propagating in the material. This is especially important for transient signals, where not only the long-living eigenmodes contribute to the sound radiation. Our analyses support that piezopolymer sensors can be employed as a general tool for the determination of the internal dynamics of vibrating systems.
We study dynamics of populations of resonantly coupled oscillators having different frequencies. Starting from the coupled van der Pol equations we derive the Kuramoto-type phase model for the situation, where the natural frequencies of two interacting subpopulations are in relation 2 : 1. Depending on the parameter of coupling, ensembles can demonstrate fully synchronous clusters, partial synchrony (only one subpopulation synchronizes), or asynchrony in both subpopulations. Theoretical description of the dynamics based on the Watanabe-Strogatz approach is developed.
We propose a novel method of reconstructing the topology and interaction functions for a general oscillator network. An ensemble of initial phases and the corresponding instantaneous frequencies is constructed by repeating random phase resets of the system dynamics. The desired details of network structure are then revealed by appropriately averaging over the ensemble. The method is applicable for a wide class of networks with arbitrary emergent dynamics, including full synchrony.
Control of crystallographic texture from mostly face-on to edge-on is observed for the film morphology of the n-type semicrystalline polymer [N,N-9-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diy1]alt-5,59-(2,29-bithiophene)}, P(NDI2OD-T2), when annealing the film to the polymer melting point followed by slow cooling to ambient temperature. A variety of X-ray diffraction analyses, including pole figure construction and Fourier transform peak shape deconvolution, are employed to quantify the texture change, relative degree of crystallinity and lattice order. We find that annealing the polymer film to the melt leads to a shift from 77.5% face-on to 94.6% edge-on lamellar texture as well as to a 2-fold increase in crystallinity and a 40% decrease in intracrystallite cumulative disorder. The texture change results in a significant drop in the electron-only diode current density through the film thickness upon melt annealing while little change is observed in the in-plane transport of bottom gated thin film transistors. This suggests that the texture change is prevalent in the film interior and that either the (bottom) surface structure is different from the interior structure or the intracrystalline order and texture play a secondary role in transistor transport for this material.
This study uses an in vitro rd10 mouse model to quantify and compare the ability of the monopolar and the (concentric) bipolar electrode configurations for subretinal stimulation. To allow for results which can be directly compared an identical region of the retina was stimulated due to the circumstance that the bipolar electrode configuration allows also for monopolar stimulation, if the concentric counter-electrode is set potential-free (floating). A ganglion cell, located centrally over the bipolar electrode configuration was selected to extracellularly record action potentials during stimulation. To analyse the recorded action potentials, we introduce a new method which combines the advantages of (a) singular value decomposition (SVD) for weighting similar modulation patterns with which the recorded action potentials are characterized and (b) multi curve fitting to identify a common threshold level, required to finally assemble a strength-duration relationship (SDR). By directly comparing the obtained SDR curves, we found that the efficiency of stimulation with the monopolar electrode configuration is significantly higher than with the bipolar electrode configuration. All obtained SDR curves were fitted using the Lapicque model to estimate the chronaxie times and the rheobase currents. Liquid inclusions, eventually separating the retina from the electrodes are discussed to be a major cause for low ganglion cell responses during stimulation with the bipolar electrode configuration.
Cellular polypropylene (PP) ferroelectrets combine a large piezoelectricity with mechanical flexibility and elastic compliance. Their charging process represents a series of dielectric barrier discharges (DBDs) that generate a cold plasma with numerous active species and thus modify the inner polymer surfaces of the foam cells. Both the threshold for the onset of DBDs and the piezoelectricity of ferroelectrets are sensitive to repeated DBDs in the voids. It is found that the threshold voltage is approximately halved and the charging efficiency is clearly improved after only 10(3) DBD cycles. However, plasma modification of the inner surfaces from repeated DBDs deteriorates the chargeability of the voids, leading to a significant reduction of the piezoelectricity in ferroelectrets. After a significant waiting period, the chargeability of previously fatigued voids shows a partial recovery. The plasma modification is, however, detrimental to the stability of the deposited charges and thus also of the macroscopic dipoles and of the piezoelectricity. Fatigue from only 10(3) DBD cycles already results in significantly less stable piezoelectricity in cellular PP ferroelectrets. The fatigue rate as a function of the number of voltage cycles follows a stretched exponential. Fatigue from repeated DBDs can be avoided if most of the gas molecules inside the voids are removed via a suitable evacuation process.
We consider general properties of groups of interacting oscillators, for which the natural frequencies are not in resonance. Such groups interact via nonoscillating collective variables like the amplitudes of the order parameters defined for each group. We treat the phase dynamics of the groups using the Ott-Antonsen ansatz and reduce it to a system of coupled equations for the order parameters. We describe different regimes of cosynchrony in the groups. For a large number of groups, heteroclinic cycles, corresponding to a sequential synchronous activity of groups and chaotic states where the order parameters oscillate irregularly, are possible.
Photo-induced deformations in azobenzene-containing polymers (azo-polymers) are central to a number of applications, such as optical storage and fabrication of diffractive elements. The microscopic nature of the underlying opto-mechanical coupling is yet not clear. In this study, we address the experimental finding that the scenario of the effects depends on molecular architecture of the used azo-polymer. Typically, opposite deformations in respect to the direction of light polarization are observed for liquid crystalline and amorphous azo-polymers. In this study, we undertake molecular dynamics simulations of two different models that mimic these two types of azo-polymers. We employ hybrid force field modeling and consider only trans-isomers of azobenzene, represented as Gay-Berne sites. The effect of illumination on the orientation of the chromophores is considered on the level of orientational hole burning and emphasis is given to the resulting deformation of the polymer matrix. We reproduce deformations of opposite sign for the two models being considered here and discuss the relevant microscopic mechanisms in both cases.
The collective dynamics of oscillator networks with phase-repulsive coupling is studied, considering various network sizes and topologies. The notion of link frustration is introduced to characterize and quantify the network dynamical states. In opposition to widely studied phase-attractive case, the properties of final dynamical states in our model critically depend on the network topology. In particular, each network's total frustration value is intimately related to its topology. Moreover, phase-repulsive networks in general display multiple final frustration states, whose statistical and stability properties are uniquely identifying them.
Within the Schwinger-Keldysh formalism we derive a Ginzburg-Landau theory for the Bose-Hubbard model which describes the real-time dynamics of the complex order parameter field. Analyzing the excitations in the vicinity of the quantum phase transitions it turns out that particle/hole dispersions in the Mott phase map continuously onto corresponding amplitude/phase excitations in the superfluid phase. Furthermore, in the superfluid phase we find a sound mode, which is in accordance with recent Bragg spectroscopy measurements in the Bogoliubov regime, as well as an additional gapped mode, which seems to have been detected via lattice modulation.
We present a new approach to observationally constraining the spectral energy distribution of the intergalactic UV background by studying metal absorption systems. We study single-component metal line systems that exhibit various well-measured species. Among the observed transitions, at least two ratios of ionization stages from the same element are required, e. g. C III/C IV and Si III/Si IV. For each system photoionization models are constructed by varying the spectrum of the ionizing radiation. The spectral energy distribution can then be constrained by comparing the models with the observed column density ratios. Extensive tests with artificial absorbers show that the spectrum of the ionizing radiation cannot be reconstructed unambiguously, but it is possible to constrain the main characteristics of the spectrum. Furthermore, the resulting physical parameters of the absorber, such as ionization parameter, metallicity, and relative abundances, may depend strongly on the adopted ionizing spectrum. Even in case of well-fitting models, the uncertainties can be as high as similar to 0.5 dex for the ionization parameter and up to similar to 1.5 dex for the metallicity. Therefore, it is essential to know the hardness of the UV background when estimating the metallicity of the intergalactic medium. Applying the procedure to a small sample of 3 observed single-component metal line systems yields a soft ionizing radiation at z > 2 and a slightly harder spectrum at z < 2. The resulting energy distributions exhibit strong He II Lya re-emission features, suggesting that reprocessing by intergalactic He II is important. Comparing the observed systems to UV background spectra from the literature indicates that a recent model that includes sawtooth modulation due to reprocessing by intergalactic He II with delayed helium reionization fits the investigated systems very well.
New materials for polymer organic light-emitting diodes based on a polymer matrix doped with phosphorescent dyes are presented. The matrix system is based on a polystyrene backbone bearing either electron or hole transporting units at the 4-position of each repeat unit. Random copolymers and polymer blend systems of the homopolymers are prepared, both with 62 wt.% electron transporting and 38 wt.% hole transporting moieties. Adding a green electrophosphorescent dye to the polymer matrix leads to efficient electroluminescence with a maximum current efficiency of 35 cd/A and a maximum external quantum efficiency of up to 10%. The mobilities of electrons and holes in the dye-doped copolymer, as measured by transient electroluminescence, are around 5 x 10(-5) and 5 x 10(-6) cm(2)/Vs, respectively, while the blend of the two homopolymers exhibits slightly lower mobilities of both types of carriers. Despite the pronounced imbalance of charge transport, the device performance is almost entirely limited by the phosphorescence efficiency of the dye, implying balanced flow of holes and electrons into the active region. Also, devices made with either the copolymer or the blend yielded very similar device efficiencies, despite the noticeable difference in electron and hole mobility. It is proposed that electrons are efficiently blocked at the interlayer and that the so-formed space charge assists the balanced injection of holes.
We present a general formulation of Floquet states of periodically time-dependent open Markovian quasifree fermionic many-body systems in terms of a discrete Lyapunov equation. Illustrating the technique, we analyze periodically kicked XY spin-1/2 chain which is coupled to a pair of Lindblad reservoirs at its ends. A complex phase diagram is reported with reentrant phases of long range and exponentially decaying spin-spin correlations as some of the system's parameters are varied. The structure of phase diagram is reproduced in terms of counting nontrivial stationary points of Floquet quasiparticle dispersion relation.
We report on the interaction of cationic azobenzene-containing surfactant with DNA investigated by absorption and fluorescence spectroscopy, dynamic light scattering, and atomic force microscopy. The properties of the surfactant can be controlled with light by reversible switching of the azobenzene unit, incorporated into the surfactant tail, between a hydrophobic trans (visible irradiation) and a hydrophilic cis (UV irradiation) configuration. The influence of the trans-cis isomerization of the azobenzene on the compaction process of DNA molecules and the role of both isomers in the formation and colloidal stability of DNA-surfactant complexes is discussed. It is shown that the trans isomer plays a major role in the DNA compaction process. The influence of the cis isomer on the DNA coil configuration is rather small. The construction of a phase diagram of the DNA concentration versus surfactant/DNA charge ratio allows distancing between three major phases: colloidally stable and unstable compacted globules, and extended coil conformation. There is a critical concentration of DNA above which the compacted globules can be hindered from aggregation and precipitation by adding an appropriate amount of the surfactant in the trans configuration. This is because of the compensation of hydrophobicity of the globules with an increasing amount of the surfactant. Below the critical DNA concentration, the compacted globules are colloidally stable and can be reversibly transferred with light to an extended coil state.
Change points in time series are perceived as isolated singularities where two regular trends of a given signal do not match. The detection of such transitions is of fundamental interest for the understanding of the system's internal dynamics or external forcings. In practice observational noise makes it difficult to detect such change points in time series. In this work we elaborate on a Bayesian algorithm to estimate the location of the singularities and to quantify their credibility. We validate the performance and sensitivity of our inference method by estimating change points of synthetic data sets. As an application we use our algorithm to analyze the annual flow volume of the Nile River at Aswan from 1871 to 1970, where we confirm a well-established significant transition point within the time series.