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Adsorption of amino acids on the magnetite-(111)-surface: a force field study (vol 19, 851, 2013)
(2016)
Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics
(2016)
Ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbital and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)(5) in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given-which will be covered experimentally by upcoming transform-limited x-ray sources.
p-Type Doping of Poly(3-hexylthiophene) with the Strong Lewis Acid Tris(pentafluorophenyl)borane
(2016)
State-of-the-art p-type doping of organic semiconductors is usually achieved by employing strong -electron acceptors, a prominent example being tetrafluorotetracyanoquinodimethane (F(4)TCNQ). Here, doping of the semiconducting model polymer poly(3-hexylthiophene), P3HT, using the strong Lewis acid tris(pentafluorophenyl)borane (BCF) as a dopant, is investigated by admittance, conductivity, and electron paramagnetic resonance measurements. The electrical characteristics of BCF- and F(4)TCNQ-doped P3HT layers are shown to be very similar in terms of the mobile hole density and the doping efficiency. Roughly 18% of the employed dopants create mobile holes in either F-4 TCNQ- or BCF-doped P3HT, while the majority of doping-induced holes remain strongly Coulomb-bound to the dopant anions. Despite similar hole densities, conductivity and hole mobility are higher in BCF-doped P3HT layers than in F(4)TCNQ-doped samples. This and the good solubility in many organic solvents render BCF very useful for p-type doping of organic semiconductors.
A dual-characteristic polymer field-effect transistor has markedly different characteristics in low and high voltage operations. In the low-voltage range (<5 V) it shows sharp subthreshold slopes (0.3–0.4 V dec−1), using which a low-voltage inverter with gain 8 is realized, while high-voltage (>5 V) induces symmetric current with regard to drain and gate voltages, leading to discrete differential (trans) conductances.
A synchronization experiment on two mutual interacting organ pipes is compared with a theoretical model which takes into account the coupling mechanisms by the underlying first principles of fluid mechanics and aeroacoustics. The focus is on the Arnold-tongue, a mathematical object in the parameter space of detuning and coupling strength which quantitatively captures the interaction of the synchronized sound sources. From the experiment, a nonlinearly shaped Arnold-tongue is obtained, describing the coupling of the synchronized pipe-pipe system. This is in contrast to the linear shaped Arnold-tongue found in a preliminary experiment of the coupled system pipe-loudspeaker. To understand the experimental result, a coarse-grained model of two nonlinear coupled self-sustained oscillators is developed. The model, integrated numerically, is in very good agreement with the synchronization experiment for separation distances of the pipes in the far field and in the intermediate field. The methods introduced open the door for a deeper understanding of the fundamental processes of sound generation and the coupling mechanisms on mutual interacting acoustic oscillators. (C) 2016 Acoustical Society of America.
The very high energy (VHE; E > 100 GeV) blazar Markarian 501 was observed between April 17 and May 5 (MJD 54 938-54 956), 2009, as part of an extensive multiwavelength campaign from radio to VHE. Strong VHE yray activity was detected on May 1st with Whipple and VERITAS, when the flux (E > 400 GeV) increased to 10 times the preflare baseline flux (3.9 x 10(-11) ph cm(-2) s(-1)), reaching five times the flux of the Crab Nebula. This coincided with a decrease in the optical polarization and a rotation of the polarization angle by 15. This VHE flare showed a fast flux variation with an increase of a factor similar to 4 in 25 min, and a falling time of similar to 50 min. We present the observations of the quiescent state previous to the flare and of the high state after the flare, focusing on the flux and spectral variability from Whipple, VERITAS, Fermi-LAT, RXTE, and Swift combined with optical and radio data.
The density of firn is an important property for monitoring and modeling the ice sheets as well as to model the pore close-off and thus to interpret ice core-based greenhouse gas records. One feature, which is still in debate, is the potential existence of an annual cycle of firn density in low-accumulation regions. Several studies describe or assume seasonally successive density layers, horizontally evenly distributed, as seen in radar data. On the other hand, high-resolution density measurements on firn cores in Antarctica and Greenland show no clear seasonal cycle in the top few meters. A major caveat of most existing snow-pit and firn-core-based studies is that they represent one vertical profile from a laterally heterogeneous density field. To overcome this, we created an extensive data set of horizontal and vertical density data at Kohnen Station, Dronning Maud Land, on the East Antarctic Plateau. We drilled and analyzed three 90m long firn cores as well as 143 one-meter-long vertical profiles from two elongated snow trenches to obtain a two-dimensional view of the density variations. The analysis of the 45m wide and 1m deep density fields reveals a seasonal cycle in density. However, the seasonality is overprinted by strong stratigraphic noise, making it invisible when analyzing single firn cores. Our density data set extends the view from the local ice core perspective to a hundred meter scale and thus supports linking spatially integrating methods such as radar and seismic studies to ice and firn cores.
Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 angstrom and temporal resolution of 230 fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.
X-ray free electron lasers (XFELs) enable unprecedented new ways to study the electronic structure and dynamics of transition metal systems. L-edge absorption spectroscopy is a powerful technique for such studies and the feasibility of this method at XFELs for solutions and solids has been demonstrated. However, the required x-ray bandwidth is an order of magnitude narrower than that of self-amplified spontaneous emission (SASE), and additional monochromatization is needed. Here we compare L-edge x-ray absorption spectroscopy (XAS) of a prototypical transition metal system based on monochromatizing the SASE radiation of the linac coherent light source (LCLS) with a new technique based on self-seeding of LCLS. We demonstrate how L-edge XAS can be performed using the self-seeding scheme without the need of an additional beam line monochromator. We show how the spectral shape and pulse energy depend on the undulator setup and how this affects the x-ray spectroscopy measurements. (C) 2016 Optical Society of America
A search for dark matter linelike signals iss performed in the vicinity of the Galactic Center by the H.E.S.S. experiment on observational data taken in 2014. An unbinned likelihood analysis iss developed to improve the sensitivity to linelike signals. The upgraded analysis along with newer data extend the energy coverage of the previous measurement down to 100 GeV. The 18 h of data collected with the H.E.S.S. array allow one to rule out at 95% C.L. the presence of a 130 GeV line (at l = -1.5 degrees, b = 0 degrees and for a dark matter profile centered at this location) previously reported in Fermi-LAT data. This new analysis overlaps significantly in energy with previous Fermi-LAT and H.E.S.S. results. No significant excess associated with dark matter annihilations was found in the energy range of 100 GeV to 2 TeV and upper limits on the gamma-ray flux and the velocity weighted annihilation cross section are derived adopting an Einasto dark matter halo profile. Expected limits for present and future large statistics H.E.S.S. observations are also given.
In this Comment, we review the results of pattern formation in a reaction-diffusion-advection system following the kinetics of the Gray-Scott model. A recent paper by Das [Phys. Rev. E 92, 052914 (2015)] shows that spatiotemporal chaos of the intermittency type can disappear as the advective flow is increased. This study, however, refers to a single point in the space of kinetic parameters of the original Gray-Scott model. Here we show that the wealth of patterns increases substantially as some of these parameters are changed. In addition to spatiotemporal intermittency, defect-mediated turbulence can also be found. In all cases, however, the chaotic behavior is seen to disappear as the advective flow is increased, following a scenario similar to what was reported in our earlier work [I. Berenstein and C. Beta, Phys. Rev. E 86, 056205 (2012)] as well as by Das. We also point out that a similar phenomenon can be found in other reaction-diffusion-advection models, such as the Oregonator model for the Belousov-Zhabotinsky reaction under flow conditions.
Sunspot positions from various historical sets of solar drawings are analyzed with respect to the tilt angles of bipolar sunspot groups. Data by Scheiner, Hevelius, Staudacher, Zucconi, Schwabe, and Sporer deliver a series of average tilt angles spanning a period of 270 years, additional to previously found values for 20th-century data obtained by other authors. We find that the average tilt angles before the Maunder minimum were not significantly different from the modem values. However, the average tilt angles of a period 50 years after the Maunder minimum, namely for cycles 0 and 1, were much lower and near zero. The normal tilt angles before the Maunder minimum suggest that it was not abnormally low tilt angles which drove the solar cycle into a grand minimum. (C) 2016 COSPAR. Published by Elsevier Ltd. All rights reserved.
We discuss the failure of the Markov approximation in the description of atom-surface fluctuation-induced interactions, both in equilibrium (Casimir-Polder forces) and out of equilibrium (quantum friction). Using general theoretical arguments, we show that the Markov approximation can lead to erroneous predictions of such phenomena with regard to both strength and functional dependencies on system parameters. In particular, we show that the long-time power-law tails of two-time dipole correlations and their corresponding low-frequency behavior, neglected in the Markovian limit, affect the prediction of the force. Our findings highlight the importance of non-Markovian effects in dispersion interactions.
We study the z approximate to 3.5 intergalactic medium (IGM) by comparing new, high-quality absorption spectra of eight QSOs with < z(QSO)> = 3.75, to virtual observations of the Evolution and Assembly of Galaxies and their Environments (EAGLE) cosmological hydrodynamical simulations. We employ the pixel optical depth method and uncover strong correlations between various combinations of H I, C III, C IV, Si III, Si IV, and O VI. We find good agreement between many of the simulated and observed correlations, including tau(O) (VI) (tau(H) (I)). However, the observed median optical depths for the tau(C) (IV) (tau(H) (I)) and tau(Si) (IV) (tau(H) (I)) relations are higher than those measured from the mock spectra. The discrepancy increases from up to approximate to 0.1 dex at tau(H) (I) = 1 to approximate to 1 dex at tau(H) (I) = 10(2), where we are likely probing dense regions at small galactocentric distances. As possible solutions, we invoke (a) models of ionizing radiation softened above 4 Ryd to account for delayed completion of He II reionization; (b) simulations run at higher resolution; (c) the inclusion of additional line broadening due to unresolved turbulence; and (d) increased elemental abundances; however, none of these factors can fully explain the observed differences. Enhanced photoionization of H I by local sources, which was not modelled, could offer a solution. However, the much better agreement with the observed O VI(H I) relation, which we find probes a hot and likely collisionally ionized gas phase, indicates that the simulations are not in tension with the hot phase of the IGM, and suggests that the simulated outflows may entrain insufficient cool gas.
The spatial and temporal control over presentation of protein-based biomolecules such as growth factors and hormones is crucial for in vitro applications to mimic the complex in vivo environment. We investigated the interaction of a model protein lysozyme (Lys) with poly(L-lysine)/hyaluronic acid (PLL/HA) multilayer films. We focused on Lys diffusion as well as adsorption and retention within the film as a function of the film deposition conditions and post-treatment. Additionally, an effect of Lys concentration on its mobility was probed. A combination of confocal fluorescence microscopy, fluorescence recovery after photobleaching, and microfluidics was employed for this investigation. Our main finding is that adsorption of PLL and HA after protein loading induces acceleration and reduction of Lys mobility, respectively. These results suggest that a charge balance in the film to a high extent governs the protein-film interaction. We believe that control over protein mobility is a key to reach the full potential of the PLL/HA films as reservoirs for biomolecules depending on the application demand. (C) 2016 The Authors. Published by Elsevier B.V.
Massive stars are extremely luminous and drive strong winds, blowing a large part of their matter into the galactic environment before they finally explode as a supernova. Quantitative knowledge of massive star feedback is required to understand our Universe as we see it. Traditionally, massive stars have been studied under the assumption that their winds are homogeneous and stationary, largely relying on the Sobolev approximation. However, Observations with the newest instruments, together with progress in model calculations, ultimately dictate a cardinal change of this paradigm: stellar winds are highly inhomogeneous. Hence, we are now advancing to a new stage in our understanding of stellar winds. Using the foundations laid by V.V. Sobolev and his school, we now update and further develop the stellar spectral analysis techniques. New sophisticated 3-D models of radiation transfer in inhomogeneous expanding media elucidate the physics of stellar winds and improve classical empiric mass-loss rate diagnostics. Applications of these new techniques to multiwavelength observations of massive stars yield consistent and robust stellar wind parameters. (C) 2016 Elsevier Ltd. All rights reserved.
We study the properties of ageing Scher-Montroll transport in terms of a biased subdiffusive continuous time random walk in which the waiting times between consecutive jumps of the charge carriers are distributed according to the power law probability with . As we show, the dynamical properties of the Scher-Montroll transport depend on the ageing time span between the initial preparation of the system and the start of the observation. The Scher-Montroll transport theory was originally shown to describe the photocurrent in amorphous solids in the presence of an external electric field, but it has since been used in many other fields of physical sciences, in particular also in the geophysical context for the description of the transport of tracer particles in subsurface aquifers. In the absence of ageing () the photocurrent of the classical Scher-Montroll model or the breakthrough curves in the groundwater context exhibit a crossover between two power law regimes in time with the scaling exponents and . In the presence of ageing a new power law regime and an initial plateau regime of the current emerge. We derive the different power law regimes and crossover times of the ageing Scher-Montroll transport and show excellent agreement with simulations of the process. Experimental data of ageing Scher-Montroll transport in polymeric semiconductors are shown to agree well with the predictions of our theory.
Methods. In most cases, the given orientation of the ecliptic is used to set up the heliographic coordinate system for the drawings. Positions and sizes are measured manually on screen. Very early drawings have no indication of their orientation. A rotational matching using common spots of adjacent days is used in some cases, while in other cases, the assumption that images were aligned with a zenith-horizon coordinate system appeared to be the most probable.
Talbot-Lau interferometry provides X-ray imaging techniques with significant enhancement of the radiographic contrast of weakly absorbing objects. The grating based technique allows separation of absorption, refraction and small angle scattering effects. The different efficiency of rectangular and triangular shaped phase gratings at varying detector distances is investigated. The interference patterns (Talbot carpets) are modeled for parallel monochromatic radiation and measured by synchrotron radiation. In comparison to rectangular shapes of phase gratings much higher visibility is obtained for triangular shapes which yield enhanced contrast of a glass capillary test specimen.
In this study we present analytical solutions for convection and diffusion equations. We gather here the analytical solutions for the one-dimensional convection equation, the two-dimensional convection problem, and the one- and two-dimensional diffusion equations. Using obtained analytical solutions, we test the four-dimensional Versatile Electron Radiation Belt code (the VERB-4D code), which solves the modified Fokker-Planck equation with additional convection terms. The ninth-order upwind numerical scheme for the one-dimensional convection equation shows much more accurate results than the results obtained with the third-order scheme. The universal limiter eliminates unphysical oscillations generated by high-order linear upwind schemes. Decrease in the space step leads to convergence of a numerical solution of the two-dimensional diffusion equation with mixed terms to the analytical solution. We compare the results of the third- and ninth-order schemes applied to magnetospheric convection modeling. The results show significant differences in electron fluxes near geostationary orbit when different numerical schemes are used.
Improved measurements of the photospheric and chromospheric three-dimensional magnetic and flow fields are crucial for a precise determination of the origin and evolution of active regions. We present an illustrative sample of multi-instrument data acquired during a two-week coordinated observing campaign in August 2015 involving, among others, the GREGOR solar telescope (imaging and near-infrared spectroscopy) and the space missions Solar Dynamics Observatory (SDO) and Interface Region Imaging Spectrograph (IRIS). The observations focused on the trailing part of active region NOAA 12396 with complex polarity inversion lines and strong intrusions of opposite polarity flux. The GREGOR Infrared Spectrograph (GRIS) provided Stokes IQUV spectral profiles in the photospheric Si i.1082.7 nm line, the chromospheric He I lambda 1083.0 nm triplet, and the photospheric Ca I lambda 1083.9 nm line. Carefully calibrated GRIS scans of the active region provided maps of Doppler velocity and magnetic field at different atmospheric heights. We compare quick-look maps with those obtained with the " Stokes Inversions based on Response functions" (SIR) code, which furnishes deeper insight into the magnetic properties of the region. We find supporting evidence that newly emerging flux and intruding opposite polarity flux are hampering the formation of penumbrae, i.e., a penumbra fully surrounding a sunspot is only expected after cessation of flux emergence in proximity to the sunspots. (C) 2016 WILEY-VCH Verlag GmbH& Co.KGaA, Weinheim
The new generation of solar instruments provides better spectral, spatial, and temporal resolution for a better understanding of the physical processes that take place on the Sun. Multiple-component profiles are more commonly observed with these instruments. Particularly, the He i 10830 triplet presents such peculiar spectral profiles, which give information on the velocity and magnetic fine structure of the upper chromosphere. The purpose of this investigation is to describe a technique to efficiently fit the two blended components of the He i 10830 triplet, which are commonly observed when two atmospheric components are located within the same resolution element. The observations used in this study were taken on 2015 April 17 with the very fast spectroscopic mode of the GREGOR Infrared Spectrograph (GRIS) attached to the 1.5-m GREGOR solar telescope, located at the Observatorio del Teide, Tenerife, Spain. We apply a double-Lorentzian fitting technique using Levenberg-Marquardt least-squares minimization. This technique is very simple and much faster than inversion codes. Line-of-sight Doppler velocities can be inferred for a whole map of pixels within just a few minutes. Our results show sub-and supersonic downflow velocities of up to 32 km s(-1) for the fast component in the vicinity of footpoints of filamentary structures. The slow component presents velocities close to rest. (C) 2016 WILEY-VCH Verlag GmbH& Co. KGaA, Weinheim
Arch filament systems occur in active sunspot groups, where a fibril structure connects areas of opposite magnetic polarity, in contrast to active region filaments that follow the polarity inversion line. We used the GREGOR Infrared Spectrograph (GRIS) to obtain the full Stokes vector in the spectral lines SiI lambda 1082.7 nm, He I lambda 1083.0 nm, and Ca I lambda 1083.9 nm. We focus on the near-infrared calcium line to investigate the photospheric magnetic field and velocities, and use the line core intensities and velocities of the helium line to study the chromospheric plasma. The individual fibrils of the arch filament system connect the sunspot with patches of magnetic polarity opposite to that of the spot. These patches do not necessarily coincide with pores, where the magnetic field is strongest. Instead, areas are preferred not far from the polarity inversion line. These areas exhibit photospheric downflows of moderate velocity, but significantly higher downflows of up to 30 km s(-1) in the chromospheric helium line. Our findings can be explained with new emerging flux where the matter flows downward along the field lines of rising flux tubes, in agreement with earlier results. (C) 2016 WILEY-VCH Verlag GmbH& Co. KGaA, Weinheim
The strong adhesion of sub-micron sized particles to surfaces is a nuisance, both for removing contaminating colloids from surfaces and for conscious manipulation of particles to create and test novel micro/nano-scale assemblies. The obvious idea of using detergents to ease these processes suffers from a lack of control: the action of any conventional surface-modifying agent is immediate and global. With photosensitive azobenzene containing surfactants we overcome these limitations. Such photo-soaps contain optical switches (azobenzene molecules), which upon illumination with light of appropriate wavelength undergo reversible trans-cis photo-isomerization resulting in a subsequent change of the physico-chemical molecular properties. In this work we show that when a spatial gradient in the composition of trans-and cis-isomers is created near a solid-liquid interface, a substantial hydrodynamic flow can be initiated, the spatial extent of which can be set, e.g., by the shape of a laser spot. We propose the concept of light induced diffusioosmosis driving the flow, which can remove, gather or pattern a particle assembly at a solid-liquid interface. In other words, in addition to providing a soap we implement selectivity: particles are mobilized and moved at the time of illumination, and only across the illuminated area.
On the basis of the layer-by-layer deposition of polyelectrolytes, we have designed hybrid nanolayer composites for integrated optoacoustic experiments. The femtosecond-laser-excitation of an Azo functionalized film launches nanoscale strain waves at GHz frequencies into a transparent polymer layer. Gold nanorods deposited on the surface sense the arrival of these hyper-sound-waves on the picosecond time scale via a modification of their longitudinal plasmon resonance. We simulated the strain waves using a simple linear masses-and-springs model, which yields good agreement with the observed time scales associated with the nanolayer thicknesses of the constituent materials. From systematic experiments with calibrated strain amplitudes we conclude that reversible viscoelastic deformations of the polyelectrolyte multilayers are triggered by ultrashort pressure transients of about 4 MPa. Our experiments show that strain-mediated interactions in nanoarchitectures composed of molecular photoswitches and plasmonic particles may be used to design new functionalities. The approach combines the highly flexible and cost-effective preparation of polyelectrolyte multilayers with ultrafast molecular strain actuation and plasmonic sensing. Although we use simple flat layered structures for demonstration, this new concept can be used for three-dimensional nanoassemblies with different functionalities. The ultrafast and reversible nature of the response is highly desirable, and the short wavelength associated with the high frequency of the hyper-sound-waves connecting photoactive molecules and nanoparticles inherently gives spectroscopic access to the nanoscale. High-frequency elastic moduli are derived from the ultrafast spectroscopy of the hypersonic response in polyelectrolyte multilayers.
A SEARCH FOR VERY HIGH ENERGY GAMMA RAYS FROM THE MISSING LINK BINARY PULSAR J1023+0038 WITH VERITAS
(2016)
The binary millisecond radio pulsar PSR J1023+0038 exhibits many characteristics similar to the gamma-ray binary system PSR B1259-63/LS 2883, making it an ideal candidate for the study of high-energy nonthermal emission. It has been the subject of multiwavelength campaigns following the disappearance of the pulsed radio emission in 2013 June, which revealed the appearance of an accretion disk around the neutron star. We present the results of very high energy (VHE) gamma-ray observations carried out by the Very Energetic Radiation Imaging Telescope Array System before and after this change of state. Searches for steady and pulsed emission of both data sets yield no significant gamma-ray signal above 100 GeV, and upper limits are given for both a steady and pulsed gamma-ray flux. These upper limits are used to constrain the magnetic field strength in the shock region of the PSR J1023+0038 system. Assuming that VHE gamma rays are produced via an inverse Compton mechanism in the shock region, we constrain the shock magnetic field to be greater than similar to 2 G before the disappearance of the radio pulsar and greater than similar to 10 G afterward.
A recently reported novel class of elastomers was tested with respect to its dielectric properties. The new elastomer material is based on a commercially available poly(dimethylsiloxane) composition, which has been modified by embedding glycerol droplets into its matrix. The approach has two major advantages that make the material useful in a dielectric actuator. First, the glycerol droplets efficiently enhance the dielectric constant, which can reach astonishingly high values in the composite. Second, the liquid filler also acts as a softener that effectively decreases the elastic modulus of the composite. In combination with very low cost and easy preparation, the two property enhancements lead to an extremely attractive dielectric elastomer material. Experimental permittivity data are compared to various theoretical models that predict relative permittivity changes as a function of filler loading, and the applicability of the models is discussed. (c) 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 44153.
The competition between charge extraction and nongeminate recombination critically determines the current-voltage characteristics of organic solar cells (OSCs) and their fill factor. As a measure of this competition, several figures of merit (FOMs) have been put forward; however, the impact of space charge effects has been either neglected, or not specifically addressed. Here we revisit recently reported FOMs and discuss the role of space charge effects on the interplay between recombination and extraction. We find that space charge effects are the primary cause for the onset of recombination in so-called non-Langevin systems, which also depends on the slower carrier mobility and recombination coefficient. The conclusions are supported with numerical calculations and experimental results of 25 different donor/acceptor OSCs with different charge transport parameters, active layer thicknesses or composition ratios. The findings represent a conclusive understanding of bimolecular recombination for drift dominated photocurrents and allow one to minimize these losses for given device parameters.
When does a diffusing particle reach its target for the first time? This first-passage time (FPT) problem is central to the kinetics of molecular reactions in chemistry and molecular biology. Here, we explain the behavior of smooth FPT densities, for which all moments are finite, and demonstrate universal yet generally non-Poissonian long-time asymptotics for a broad variety of transport processes. While Poisson-like asymptotics arise generically in the presence of an effective repulsion in the immediate vicinity of the target, a time-scale separation between direct and reflected indirect trajectories gives rise to a universal proximity effect: Direct paths, heading more or less straight from the point of release to the target, become typical and focused, with a narrow spread of the corresponding first-passage times. Conversely, statistically dominant indirect paths exploring the entire system tend to be massively dissimilar. The initial distance to the target particularly impacts gene regulatory or competitive stochastic processes, for which few binding events often determine the regulatory outcome. The proximity effect is independent of details of the transport, highlighting the robust character of the FPT features uncovered here.
We present a nanostructured device that functions as photoacoustic hard x-ray switch. The device is triggered by femtosecond laser pulses and allows for temporal gating of hard x-rays on picosecond (ps) timescales. It may be used for pulse picking or even pulse shortening in 3rd generation synchrotron sources. Previous approaches mainly suffered from insufficient switching contrasts due to excitation-induced thermal distortions. We present a new approach where thermal distortions are spatially separated from the functional switching layers in the structure. Our measurements yield a switching contrast of 14, which is sufficient for efficient hard x-ray pulse shortening. The optimized structure also allows for utilizing the switch at high repetition rates of up to 208 kHz. Published by AIP Publishing.
Ferroelectrets are non-polar polymer foams or polymer systems with internally charged cavities. They are charged through a series of dielectric barrier discharges (DBDs) that are caused by the electrical breakdown of the gas inside the cavities. Thus, the breakdown strength of the gas strongly influences the charging process of ferroelectrets. A gas with a lower breakdown strength has a lower threshold voltage, thus decreasing the onset voltage for DBD charging. However, a lower threshold voltage also leads to a lower value for the remanent polarization, as back discharges that are caused by the electric field of the internally deposited charges can take place already at lower charge levels. On this basis, a charging strategy is proposed where the DBDs start in a gas with a lower breakdown strength (in the present example, helium) and are completed at a higher breakdown strength (e.g., nitrogen or atmospheric air). Thus, the exchange of the gas in the cavities during charging can significantly enhance the charging efficiency, i.e., yield much higher piezoelectric coefficients in ferroelectrets at significantly lower charging voltages. Published by AIP Publishing.
Effects of solvent additive on "s-shaped" curves in solution-processed small molecule solar cells
(2016)
A novel molecular chromophore, p-SIDT(FBTThCA8)(2), is introduced as an electron-donor material for bulk heterojunction (BHJ) solar cells with broad absorption and near ideal energy levels for the use in combination with common acceptor materials. It is found that films cast from chlorobenzene yield devices with strongly s-shaped current-voltage curves, drastically limiting performance. We find that addition of the common solvent additive diiodooctane, in addition to facilitating crystallization, leads to improved vertical phase separation. This yields much better performing devices, with improved curve shape, demonstrating the importance of morphology control in BHJ devices and improving the understanding of the role of solvent additives.
Hydrological and climatological controls on radiocarbon concentrations in a tropical stalagmite
(2016)
Precisely-dated stalagmites are increasingly important archives for the reconstruction of terrestrial paleoclimate at very high temporal resolution. In-depth understanding of local conditions at the cave site and of the processes driving stalagmite deposition is of paramount importance for interpreting proxy signals incorporated in stalagmite carbonate. Here we present a sub-decadally resolved dead carbon fraction (DCF) record for a stalagmite from Yok Balum Cave (southern Belize). The record is coupled to parallel stable carbon isotope (delta C-13) and U/Ca measurements, as well as radiocarbon (C-14) measurements from soils overlying the cave system. Using a karst carbon cycle model we disentangle the importance of soil and karst processes on stalagmite DCF incorporation, revealing a dominant host rock dissolution control on total DCF. Covariation between DCF, delta C-13, and U/Ca indicates that karst processes are a common driver of all three parameters, suggesting possible use of delta C-13 and trace element ratios to independently quantify DCF variability. A statistically significant multi-decadal lag of variable length exists between DCF and reconstructed solar activity, suggesting that solar activity influenced regional precipitation in Mesoamerica over the past 1500 years, but that the relationship was non-static. Although the precise nature of the observed lag is unclear, solar-induced changes in North Atlantic oceanic and atmospheric dynamics may play a role. (C) 2016 Elsevier Ltd. All rights reserved.
detected six rapid X-ray spectral hardening events called "softness dips" in a similar to 100 ks observation in 2011. All the softness dip events show symmetric softness-ratio variations, and some of them have flat bottoms apparently due to saturation. The softness dip spectra are best described by either similar to 40% or similar to 70% partial covering absorption to kT similar to 12 keV plasma emission by matter with a neutral hydrogen column density of similar to(2-8) x 10(21) cm(-2), while the spectrum outside these dips is almost free of absorption. This result suggests the presence of two distinct X-ray-emitting spots in the.. Cas system, perhaps on a white dwarf (WD) companion with dipole mass accretion. The partial covering absorbers may be blobs in the Be stellar wind, the Be disk, or rotating around the WD companion. Weak correlations of the softness ratios to the hard X-ray flux suggest the presence of stable plasmas at kT similar to 0.9 and 5 keV, which may originate from the Be or WD winds. The formation of a Be star and WD binary system requires mass transfer between two stars; gamma Cas may have experienced such activity in the past.
Fluorine-containing low-energy-gap organic dyes with low voltage losses for organic solar cells
(2016)
Fluorine-containing donor molecules TFTF, CNTF and PRTF are designed and isomer selectively synthesized for application in vacuum-deposited organic solar cells. These molecules comprise a donor acceptor molecular architecture incorporating thiophene and benzothiadiazole derivatives as the electron-donating and electron-withdrawing moieties, respectively. As opposed to previously reported materials from this class, PRTF can be purified by vacuum sublimation at moderate to high yields because of its higher volatility and better stabilization due to a stronger intramolecular hydrogen bond, as compared to TFTF and CNTF. The UV-vis absorption spectra of the three donors show an intense broadband absorption between 500 nm and 800 nm with, similar positions of their frontier energy levels. The photophysical properties of the three donor molecules are thoroughly tested and optimized in bulk heterojunction solar cells with C-60 as acceptor. PRTF shows the best performance, yielding power conversion efficiencies of up to 3.8%. Moreover, the voltage loss for the PRTF device due to the non radiative recombination of free charge carriers is exceptionally low (0.26 V) as compared to typical values for organic solar cells (>0.34V). (C) 2016 Published by Elsevier B.V.
In the study of relativistic jets one of the key open questions is their interaction with the environment on the microscopic level. Here, we study the initial evolution of both electron-proton (e(-)-p(+)) and electron-positron (e(+/-)) relativistic jets containing helical magnetic fields, focusing on their interaction with an ambient plasma. We have performed simulations of "global" jets containing helical magnetic fields in order to examine how helical magnetic fields affect kinetic instabilities such as the Weibel instability, the kinetic Kelvin-Helmholtz instability (kKHI) and the Mushroom instability (MI). In our initial simulation study these kinetic instabilities are suppressed and new types of instabilities can grow. In the e(-)-p(+) jet simulation a recollimation-like instability occurs and jet electrons are strongly perturbed. In the e(+/-) jet simulation a recollimation-like instability occurs at early times followed by a kinetic instability and the general structure is similar to a simulation without helical magnetic field. Simulations using much larger systems are required in order to thoroughly follow the evolution of global jets containing helical magnetic fields.
Context. The solar magnetic field is responsible for all aspects of solar activity. Thus, emergence of magnetic flux at the surface is the first manifestation of the ensuing solar activity. Aims. Combining high-resolution and synoptic observations aims to provide a comprehensive description of flux emergence at photospheric level and of the growth process that eventually leads to a mature active region. Methods. The small active region NOAA 12118 emerged on 2014 July 17 and was observed one day later with the 1.5-m GREGOR solar telescope on 2014 July 18. High-resolution time-series of blue continuum and G-band images acquired in the blue imaging channel (BIC) of the GREGOR Fabry-Perot Interferometer (GFPI) were complemented by synoptic line-of-sight magnetograms and continuum images obtained with the Helioseismic and Magnetic Imager (HMI) onboard the Solar Dynamics Observatory (SDO). Horizontal proper motions and horizontal plasma velocities were computed with local correlation tracking (LCT) and the differential affine velocity estimator (DAVE), respectively. Morphological image processing was employed to measure the photometric and magnetic area, magnetic flux, and the separation profile of the emerging flux region during its evolution. Results. The computed growth rates for photometric area, magnetic area, and magnetic flux are about twice as high as the respective decay rates. The space-time diagram using HMI magnetograms of five days provides a comprehensive view of growth and decay. It traces a leaf-like structure, which is determined by the initial separation of the two polarities, a rapid expansion phase, a time when the spread stalls, and a period when the region slowly shrinks again. The separation rate of 0.26 km s(-1) is highest in the initial stage, and it decreases when the separation comes to a halt. Horizontal plasma velocities computed at four evolutionary stages indicate a changing pattern of inflows. In LCT maps we find persistent flow patterns such as outward motions in the outer part of the two major pores, a diverging feature near the trailing pore marking the site of upwelling plasma and flux emergence, and low velocities in the interior of dark pores. We detected many elongated rapidly expanding granules between the two major polarities, with dimensions twice as large as the normal granules.
Context. Over the past 20 yr, the quietest areas of the solar surface have revealed a weak but extremely dynamic magnetism occurring at small scales (<500 km), which may provide an important contribution to the dynamics and energetics of the outer layers of the atmosphere. Understanding this magnetism requires the inference of physical quantities from high-sensitivity spectro-polarimetric data with high spatio-temporal resolution. Aims. We present high-precision spectro-polarimetric data with high spatial resolution (0.4") of the very quiet Sun at 1.56 mu m obtained with the GREGOR telescope to shed some light on this complex magnetism. Methods. We used inversion techniques in two main approaches. First, we assumed that the observed profiles can be reproduced with a constant magnetic field atmosphere embedded in a field-free medium. Second, we assumed that the resolution element has a substructure with either two constant magnetic atmospheres or a single magnetic atmosphere with gradients of the physical quantities along the optical depth, both coexisting with a global stray-light component. Results. Half of our observed quiet-Sun region is better explained by magnetic substructure within the resolution element. However, we cannot distinguish whether this substructure comes from gradients of the physical parameters along the line of sight or from horizontal gradients (across the surface). In these pixels, a model with two magnetic components is preferred, and we find two distinct magnetic field populations. The population with the larger filling factor has very weak (similar to 150 G) horizontal fields similar to those obtained in previous works. We demonstrate that the field vector of this population is not constrained by the observations, given the spatial resolution and polarimetric accuracy of our data. The topology of the other component with the smaller filling factor is constrained by the observations for field strengths above 250 G: we infer hG fields with inclinations and azimuth values compatible with an isotropic distribution. The filling factors are typically below 30%. We also find that the flux of the two polarities is not balanced. From the other half of the observed quiet-Sun area similar to 50% are two-lobed Stokes V profiles, meaning that 23% of the field of view can be adequately explained with a single constant magnetic field embedded in a non-magnetic atmosphere. The magnetic field vector and filling factor are reliable inferred in only 50% based on the regular profiles. Therefore, 12% of the field of view harbour hG fields with filling factors typically below 30%. At our present spatial resolution, 70% of the pixels apparently are non-magnetised.
In this paper we report on a long multi-wavelength observational campaign of the supergiant fast X-ray transient prototype IGR J17544-2619. A 150 ks-long observation was carried out simultaneously with XMM-Newton and NuSTAR, catching the source in an initial faint X-ray state and then undergoing a bright X-ray outburst lasting approximately 7 ks. We studied the spectral variability during outburst and quiescence by using a thermal and bulk Comptonization model that is typically adopted to describe the X-ray spectral energy distribution of young pulsars in high mass X-ray binaries. Although the statistics of the collected X-ray data were relatively high, we could neither confirm the presence of a cyclotron line in the broad-band spectrum of the source (0.5-40 keV), nor detect any of the previously reported tentative detections of the source spin period. The monitoring carried out with Swift/XRT during the same orbit of the system observed by XMM-Newton and NuSTAR revealed that the source remained in a low emission state for most of the time, in agreement with the known property of all supergiant fast X-ray transients being significantly sub-luminous compared to other supergiant X-ray binaries. Optical and infrared observations were carried out for a total of a few thousand seconds during the quiescence state of the source detected by XMM-Newton and NuSTAR. The measured optical and infrared magnitudes were slightly lower than previous values reported in the literature, but compatible with the known micro-variability of supergiant stars. UV observations obtained with the UVOT telescope on-board Swift did not reveal significant changes in the magnitude of the source in this energy domain compared to previously reported values.
We demonstrate in situ recorded motion of nano-objects adsorbed on a photosensitive polymer film. The motion is induced by a mass transport of the underlying photoresponsive polymer material occurring during irradiation with interference pattern. The polymer film contains azobenzene molecules that undergo reversible photoisomerization reaction from trans-to cis-conformation. Through a multi-scale chain of physico-chemical processes, this finally results in the macro-deformations of the film due to the changing elastic properties of polymer. The topographical deformation of the polymer surface is sensitive to a local distribution of the electrical field vector that allows for the generation of dynamic changes in the surface topography during irradiation with different light interference patterns. Polymer film deformation together with the motion of the adsorbed nano-particles are recorded using a homemade set-up combining an optical part for the generation of interference patterns and an atomic force microscope for acquiring the surface deformation. The particles undergo either translational or rotational motion. The direction of particle motion is towards the topography minima and opposite to the mass transport within the polymer film. The ability to relocate particles by photo-induced dynamic topography fluctuation offers a way for a non-contact simultaneous manipulation of a large number of adsorbed particles just in air at ambient conditions.
Air pollution is the number one environmental cause of premature deaths in Europe. Despite extensive regulations, air pollution remains a challenge, especially in urban areas. For studying summertime air quality in the Berlin–Brandenburg region of Germany, the Weather Research and Forecasting Model with Chemistry (WRF-Chem) is set up and evaluated against meteorological and air quality observations from monitoring stations as well as from a field campaign conducted in 2014. The objective is to assess which resolution and level of detail in the input data is needed for simulating urban background air pollutant concentrations and their spatial distribution in the Berlin–Brandenburg area. The model setup includes three nested domains with horizontal resolutions of 15, 3 and 1 km and anthropogenic emissions from the TNO-MACC III inventory. We use RADM2 chemistry and the MADE/SORGAM aerosol scheme. Three sensitivity simulations are conducted updating input parameters to the single-layer urban canopy model based on structural data for Berlin, specifying land use classes on a sub-grid scale (mosaic option) and downscaling the original emissions to a resolution of ca. 1 km × 1 km for Berlin based on proxy data including traffic density and population density. The results show that the model simulates meteorology well, though urban 2 m temperature and urban wind speeds are biased high and nighttime mixing layer height is biased low in the base run with the settings described above. We show that the simulation of urban meteorology can be improved when specifying the input parameters to the urban model, and to a lesser extent when using the mosaic option. On average, ozone is simulated reasonably well, but maximum daily 8 h mean concentrations are underestimated, which is consistent with the results from previous modelling studies using the RADM2 chemical mechanism. Particulate matter is underestimated, which is partly due to an underestimation of secondary organic aerosols. NOx (NO + NO2) concentrations are simulated reasonably well on average, but nighttime concentrations are overestimated due to the model's underestimation of the mixing layer height, and urban daytime concentrations are underestimated. The daytime underestimation is improved when using downscaled, and thus locally higher emissions, suggesting that part of this bias is due to deficiencies in the emission input data and their resolution. The results further demonstrate that a horizontal resolution of 3 km improves the results and spatial representativeness of the model compared to a horizontal resolution of 15 km. With the input data (land use classes, emissions) at the level of detail of the base run of this study, we find that a horizontal resolution of 1 km does not improve the results compared to a resolution of 3 km. However, our results suggest that a 1 km horizontal model resolution could enable a detailed simulation of local pollution patterns in the Berlin–Brandenburg region if the urban land use classes, together with the respective input parameters to the urban canopy model, are specified with a higher level of detail and if urban emissions of higher spatial resolution are used.
Interplay of coupling and common noise at the transition to synchrony in oscillator populations
(2016)
There are two ways to synchronize oscillators: by coupling and by common forcing, which can be pure noise. By virtue of the Ott-Antonsen ansatz for sine-coupled phase oscillators, we obtain analytically tractable equations for the case where both coupling and common noise are present. While noise always tends to synchronize the phase oscillators, the repulsive coupling can act against synchrony, and we focus on this nontrivial situation. For identical oscillators, the fully synchronous state remains stable for small repulsive coupling; moreover it is an absorbing state which always wins over the asynchronous regime. For oscillators with a distribution of natural frequencies, we report on a counter-intuitive effect of dispersion (instead of usual convergence) of the oscillators frequencies at synchrony; the latter effect disappears if noise vanishes.
The physical properties of galactic winds are one of the keys to understand galaxy formation and evolution. These properties can be constrained thanks to background quasar lines of sight (LOS) passing near star-forming galaxies (SFGs). We present the first results of the MusE GAs FLOw and Wind survey obtained from two quasar fields, which have eight Mg II absorbers of which three have rest equivalent width greater than 0.8 angstrom. With the new Multi Unit Spectroscopic Explorer (MUSE) spectrograph on the Very Large Telescope (VLT), we detect six (75%) Mg II host galaxy candidates within a radius of 30. from the quasar LOS. Out of these six galaxy-quasar pairs, from geometrical argument, one is likely probing galactic outflows, where two are classified as "ambiguous,"two are likely probing extended gaseous disks and one pair seems to be a merger. We focus on the wind-pair and constrain the outflow using a high-resolution quasar spectra from the Ultraviolet and Visual Echelle Spectrograph. Assuming the metal absorption to be due to ga;s flowing out of the detected galaxy through a cone along the minor axis, we find outflow velocities in the order of approximate to 150 km s(-1) (i.e., smaller than the escape velocity) with a loading factor, eta = M-out/SFR, of approximate to 0.7. We see evidence for an open conical flow, with a low-density inner core. In the future, MUSE will provide us with about 80 multiple galaxy-quasar pairs in two dozen fields.
Holographic Structuring of Elastomer Actuator: First True Monolithic Tunable Elastomer Optics
(2016)
Volume diffraction gratings (VDGs) are inscribed selectively by diffusive introduction of benzophenone and subsequent UV-holographic structuring into an electroactive dielectric elastomer actuator (DEA), to afford a continuous voltage-controlled grating shift of 17%. The internal stress coupling of DEA and optical domain allows for a new generation of true monolithic tunable elastomer optics with voltage controlled properties.