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The aim of this study was to develop a one-step synthesis of gold nanotriangles (NTs) in the presence of mixed phospholipid vesicles followed by a separation process to isolate purified NTs. Negatively charged vesicles containing AOT and phospholipids, in the absence and presence of additional reducing agents (polyampholytes, polyanions or low molecular weight compounds), were used as a template phase to form anisotropic gold nanoparticles. Upon addition of the gold chloride solution, the nucleation process is initiated and both types of particles, i.e., isotropic spherical and anisotropic gold nanotriangles, are formed simultaneously. As it was not possible to produce monodisperse nanotriangles with such a one-step procedure, the anisotropic nanoparticles needed to be separated from the spherical ones. Therefore, a new type of separation procedure using combined polyelectrolyte/micelle depletion flocculation was successfully applied. As a result of the different purification steps, a green colored aqueous dispersion was obtained containing highly purified, well-defined negatively charged flat nanocrystals with a platelet thickness of 10 nm and an edge length of about 175 nm. The NTs produce promising results in surface-enhanced Raman scattering.
In this paper two groups supporting different views on the mechanism of light induced polymer deformation argue about the respective underlying theoretical conceptions, in order to bring this interesting debate to the attention of the scientific community. The group of Prof. Nicolae Hurduc supports the model claiming that the cyclic isomerization of azobenzenes may cause an athermal transition of the glassy azobenzene containing polymer into a fluid state, the so-called photo-fluidization concept. This concept is quite convenient for an intuitive understanding of the deformation process as an anisotropic flow of the polymer material. The group of Prof. Svetlana Santer supports the re-orientational model where the mass-transport of the polymer material accomplished during polymer deformation is stated to be generated by the light-induced re-orientation of the azobenzene side chains and as a consequence of the polymer backbone that in turn results in local mechanical stress, which is enough to irreversibly deform an azobenzene containing material even in the glassy state. For the debate we chose three polymers differing in the glass transition temperature, 32 degrees C, 87 degrees C and 95 degrees C, representing extreme cases of flexible and rigid materials. Polymer film deformation occurring during irradiation with different interference patterns is recorded using a homemade set-up combining an optical part for the generation of interference patterns and an atomic force microscope for acquiring the kinetics of film deformation. We also demonstrated the unique behaviour of azobenzene containing polymeric films to switch the topography in situ and reversibly by changing the irradiation conditions. We discuss the results of reversible deformation of three polymers induced by irradiation with intensity (IIP) and polarization (PIP) interference patterns, and the light of homogeneous intensity in terms of two approaches: the re-orientational and the photo-fluidization concepts. Both agree in that the formation of opto-mechanically induced stresses is a necessary prerequisite for the process of deformation. Using this argument, the deformation process can be characterized either as a flow or mass transport.
We show that self-consistent partial synchrony in globally coupled oscillatory ensembles is a general phenomenon. We analyze in detail appearance and stability properties of this state in possibly the simplest setup of a biharmonic Kuramoto-Daido phase model as well as demonstrate the effect in limit-cycle relaxational Rayleigh oscillators. Such a regime extends the notion of splay state from a uniform distribution of phases to an oscillating one. Suitable collective observables such as the Kuramoto order parameter allow detecting the presence of an inhomogeneous distribution. The characteristic and most peculiar property of self-consistent partial synchrony is the difference between the frequency of single units and that of the macroscopic field.
Compared to their inorganic counterparts, organic semiconductors suffer from relatively low charge carrier mobilities. Therefore, expressions derived for inorganic solar cells to correlate characteristic performance parameters to material properties are prone to fail when applied to organic devices. This is especially true for the classical Shockley-equation commonly used to describe current-voltage (JV)-curves, as it assumes a high electrical conductivity of the charge transporting material. Here, an analytical expression for the JV-curves of organic solar cells is derived based on a previously published analytical model. This expression, bearing a similar functional dependence as the Shockley-equation, delivers a new figure of merit α to express the balance between free charge recombination and extraction in low mobility photoactive materials. This figure of merit is shown to determine critical device parameters such as the apparent series resistance and the fill factor.
Compared to their inorganic counterparts, organic semiconductors suffer from relatively low charge carrier mobilities. Therefore, expressions derived for inorganic solar cells to correlate characteristic performance parameters to material properties are prone to fail when applied to organic devices. This is especially true for the classical Shockley-equation commonly used to describe current-voltage (JV)-curves, as it assumes a high electrical conductivity of the charge transporting material. Here, an analytical expression for the JV-curves of organic solar cells is derived based on a previously published analytical model. This expression, bearing a similar functional dependence as the Shockley-equation, delivers a new figure of merit a to express the balance between free charge recombination and extraction in low mobility photoactive materials. This figure of merit is shown to determine critical device parameters such as the apparent series resistance and the fill factor.
The F-type star KIC. 8462852 has recently been identified as an exceptional target for search for extraterrestrial intelligence (SETI) observations. We describe an analysis methodology for optical SETI, which we have used to analyze nine hours of serendipitous archival observations of KIC. 8462852 made with the VERITAS gamma-ray observatory between 2009 and 2015. No evidence of pulsed optical beacons, above a pulse intensity at the Earth of approximately 1 photon m(-2), is found. We also discuss the potential use of imaging atmospheric Cherenkov telescope arrays in searching for extremely short duration optical transients in general.
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.
In recent decades, the Greenland Ice Sheet has been losing mass and has thereby contributed to global sea-level rise. The rate of ice loss is highly relevant for coastal protection worldwide. The ice loss is likely to increase under future warming. Beyond a critical temperature threshold, a meltdown of the Greenland Ice Sheet is induced by the self-enforcing feedback between its lowering surface elevation and its increasing surface mass loss: the more ice that is lost, the lower the ice surface and the warmer the surface air temperature, which fosters further melting and ice loss. The computation of this rate so far relies on complex numerical models which are the appropriate tools for capturing the complexity of the problem. By contrast we aim here at gaining a conceptual understanding by deriving a purposefully simple equation for the self-enforcing feedback which is then used to estimate the melt time for different levels of warming using three observable characteristics of the ice sheet itself and its surroundings. The analysis is purely conceptual in nature. It is missing important processes like ice dynamics for it to be useful for applications to sea-level rise on centennial timescales, but if the volume loss is dominated by the feedback, the resulting logarithmic equation unifies existing numerical simulations and shows that the melt time depends strongly on the level of warming with a critical slow-down near the threshold: the median time to lose 10% of the present-day ice volume varies between about 3500 years for a temperature level of 0.5 degrees C above the threshold and 500 years for 5 degrees C. Unless future observations show a significantly higher melting sensitivity than currently observed, a complete meltdown is unlikely within the next 2000 years without significant ice-dynamical contributions.
A single predator charging a herd of prey: effects of self volume and predator-prey decision-making
(2016)
We study the degree of success of a single predator hunting a herd of prey on a two-dimensional square lattice landscape. We explicitly consider the self volume of the prey restraining their dynamics on the lattice. The movement of both predator and prey is chosen to include an intelligent, decision making step based on their respective sighting ranges, the radius in which they can detect the other species (prey cannot recognise each other besides the self volume interaction): after spotting each other the motion of prey and predator turns from a nearest neighbour random walk into directed escape or chase, respectively. We consider a large range of prey densities and sighting ranges and compute the mean first passage time for a predator to catch a prey as well as characterise the effective dynamics of the hunted prey. We find that the prey's sighting range dominates their life expectancy and the predator profits more from a bad eyesight of the prey than from his own good eye sight. We characterise the dynamics in terms of the mean distance between the predator and the nearest prey. It turns out that effectively the dynamics of this distance coordinate can be captured in terms of a simple Ornstein–Uhlenbeck picture. Reducing the many-body problem to a simple two-body problem by imagining predator and nearest prey to be connected by an effective Hookean bond, all features of the model such as prey density and sighting ranges merge into the effective binding constant.
Galactic cosmic rays reach energies of at least a few petaelectronvolts (of the order of 1015 electronvolts). This implies that our Galaxy contains petaelectronvolt accelerators (‘PeVatrons’), but all proposed models of Galactic cosmic-ray accelerators encounter difficulties at exactly these energies. Dozens of Galactic accelerators capable of accelerating particles to energies of tens of teraelectronvolts (of the order of 1013 electronvolts) were inferred from recent γ-ray observations3. However, none of the currently known accelerators—not even the handful of shell-type supernova remnants commonly believed to supply most Galactic cosmic rays—has shown the characteristic tracers of petaelectronvolt particles, namely, power-law spectra of γ-rays extending without a cut-off or a spectral break to tens of teraelectronvolts4. Here we report deep γ-ray observations with arcminute angular resolution of the region surrounding the Galactic Centre, which show the expected tracer of the presence of petaelectronvolt protons within the central 10 parsecs of the Galaxy. We propose that the supermassive black hole Sagittarius A* is linked to this PeVatron. Sagittarius A* went through active phases in the past, as demonstrated by X-ray outbursts5and an outflow from the Galactic Centre6. Although its current rate of particle acceleration is not sufficient to provide a substantial contribution to Galactic cosmic rays, Sagittarius A* could have plausibly been more active over the last 106–107 years, and therefore should be considered as a viable alternative to supernova remnants as a source of petaelectronvolt Galactic cosmic rays.
Molecular signalling in living cells occurs at low copy numbers and is thereby inherently limited by the noise imposed by thermal diffusion. The precision at which biochemical receptors can count signalling molecules is intimately related to the noise correlation time. In addition to passive thermal diffusion, messenger RNA and vesicle-engulfed signalling molecules can transiently bind to molecular motors and are actively transported across biological cells. Active transport is most beneficial when trafficking occurs over large distances, for instance up to the order of 1 metre in neurons. Here we explain how intermittent active transport allows for faster equilibration upon a change in concentration triggered by biochemical stimuli. Moreover, we show how intermittent active excursions induce qualitative changes in the noise in effectively one-dimensional systems such as dendrites. Thereby they allow for significantly improved signalling precision in the sense of a smaller relative deviation in the concentration read-out by the receptor. On the basis of linear response theory we derive the exact mean field precision limit for counting actively transported molecules. We explain how intermittent active excursions disrupt the recurrence in the molecular motion, thereby facilitating improved signalling accuracy. Our results provide a deeper understanding of how recurrence affects molecular signalling precision in biological cells and novel medical-diagnostic devices.
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.
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.
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.
The general electromagnetic fluctuation theory is a powerful tool to analyze the magnetic fluctuation spectrum of a plasma. Recent works utilizing this theory for a magnetized non-relativistic isotropic Maxwellian electron-proton plasma have demonstrated that the equilibrium ratio of vertical bar delta B vertical bar/B-0 can be as high as 10(-12). This value results from the balance between spontaneous emission of fluctuations and their damping, and it is considerably smaller than the observed value vertical bar delta B vertical bar/B-0 in the solar wind at 1 au, where 10(-3) less than or similar to vertical bar delta B vertical bar/B-0 less than or similar to 10(-1). In the present manuscript, we consider an anisotropic bi-Maxwellian distribution function to investigate the effect of plasma instabilities on the magnetic field fluctuations. We demonstrate that these instabilities strongly amplify the magnetic field fluctuations and provide a sufficient mechanism to explain the observed value of vertical bar delta B vertical bar/B-0 in the solar wind at 1 au.
During the summer of 2013, a 4-month spectroscopic campaign took place to observe the variabilities in three Wolf-Rayet stars. The spectroscopic data have been analysed for WR 134 (WN6b), to better understand its behaviour and long-term periodicity, which we interpret as arising from corotating interaction regions (CIRs) in the wind. By analysing the variability of the He ii lambda 5411 emission line, the previously identified period was refined to P = 2.255 +/- 0.008 (s.d.) d. The coherency time of the variability, which we associate with the lifetime of the CIRs in the wind, was deduced to be 40 +/- 6 d, or similar to 18 cycles, by cross-correlating the variability patterns as a function of time. When comparing the phased observational grey-scale difference images with theoretical grey-scales previously calculated from models including CIRs in an optically thin stellar wind, we find that two CIRs were likely present. A separation in longitude of Delta I center dot a parts per thousand integral 90A degrees was determined between the two CIRs and we suggest that the different maximum velocities that they reach indicate that they emerge from different latitudes. We have also been able to detect observational signatures of the CIRs in other spectral lines (C iv lambda lambda 5802,5812 and He i lambda 5876). Furthermore, a DAC was found to be present simultaneously with the CIR signatures detected in the He i lambda 5876 emission line which is consistent with the proposed geometry of the large-scale structures in the wind. Small-scale structures also show a presence in the wind, simultaneously with the larger scale structures, showing that they do in fact co-exist.
Aims. Doubly ionized silicon (Si III) is a powerful tracer of diffuse ionized gas inside and outside of galaxies. It can be observed in the local Universe in ultraviolet (UV) absorption against bright extragalactic background sources. We here present an extensive study of intervening Si III-selected absorbers and study the properties of the warm circumgalactic medium (CGM) around low-redshift (z <= 0.1) galaxies. Methods. We analyzed the UV absorption spectra of 303 extragalactic background sources, as obtained with the Cosmic Origins Spectrograph (COS) on-board the Hubble Space Telescope (HST). We developed a geometrical model for the absorption-cross section of the CGM around the local galaxy population and compared the observed Si III absorption statistics with predictions provided by the model. We also compared redshifts and positions of the absorbers with those of similar to 64 000 galaxies using archival galaxy-survey data to investigate the relation between intervening Si III absorbers and the CGM. Results. Along a total redshift path of Delta z approximate to 24, we identify 69 intervening Si III systems that all show associated absorption from other low and high ions (e.g., H I, Si II, Si IV, C II, C IV). We derive a bias-corrected number density of dN/dz(Si III) = 2.5 +/- 0.4 for absorbers with column densities log N(Si III) > 12.2, which is similar to 3 times the number density of strong Mg II systems at z = 0. This number density matches the expected cross section of a Si III absorbing CGM around the local galaxy population with a mean covering fraction of < f(c)> = 0.69. For the majority (similar to 60 percent) of the absorbers, we identify possible host galaxies within 300 km s(-1) of the absorbers and derive impact parameters rho < 200 kpc, demonstrating that the spatial distributions of Si III absorbers and galaxies are highly correlated. Conclusions. Our study indicates that the majority of Si III-selected absorbers in our sample trace the CGM of nearby galaxies within their virial radii at a typical covering fraction of similar to 70 percent. We estimate that diffuse gas in the CGM around galaxies, as traced by Si III, contains substantially more (more than twice as much) baryonic mass than their neutral interstellar medium.
The slicing facility FemtoSpeX at BESSY II offers unique opportunities to study photo-induced dynamics on femtosecond time scales by means of X-ray magnetic circular dichroism, resonant and non-resonant X-ray diffraction, and X-ray absorption spectroscopy experiments in the soft X-ray regime. Besides femtosecond X-ray pulses, slicing sources inherently also produce a so-called `halo' background with a different time structure, polarization and pointing. Here a detailed experimental characterization of the halo radiation is presented, and a method is demonstrated for its correct and unambiguous removal from femtosecond time-resolved data using a special laser triggering scheme as well as analytical models. Examples are given for time-resolved measurements with corresponding halo correction, and errors of the relevant physical quantities caused by either neglecting or by applying a simplified model to describe this background are estimated.
Context. The massive Wolf-Rayet type star WR102c is located near the Quintuplet Cluster, one of the three massive star clusters in the Galactic centre region. Previous studies indicated that WR102c may have a dusty circumstellar nebula and is among the main ionising sources of the Sickle Nebula associated with the Quintuplet Cluster. Aims. The goals of our study are to derive the stellar parameters of WR102c from the analysis of its spectrum and to investigate its stellar and nebular environment. Methods. We obtained observations with the ESO VLT integral field spectrograph SINFONI in the K-band, extracted the stellar spectra, and analysed them by means of stellar atmosphere models. Results. Our new analysis supersedes the results previously reported for WR102c. We significantly decrease its bolometric luminosity and hydrogen content. We detect four early OB type stars close to WR102c. These stars have radial velocities similar to that of WR102c. We suggest that together with WR102c these stars belong to a distinct star cluster with a total mass of similar to 1000 M-circle dot. We identify a new WR nebula around WR102c in the SINFONI map of the di ff use Br gamma emission and in the HST Pa ff images. The Br gamma line at di ff erent locations is not significantly broadened and similar to the width of nebular emission elsewhere in the H i i region around WR102c. Conclusions. The massive star WR102c located in the Galactic centre region resides in a star cluster containing additional early-type stars. The stellar parameters of WR102c are typical for hydrogen-free WN6 stars. We identify a nebula surrounding WR102c that has a morphology similar to other nebulae around hydrogen-free WR stars, and propose that the formation of this nebula is linked to interaction of the fast stellar wind with the matter ejected at a previous evolutionary stage of WR102c.
We investigate the ensemble and time averaged mean squared displacements for particle diffusion in a simple model for disordered media by assuming that the local diffusivity is both fluctuating in time and has a deterministic average growth or decay in time. In this study we compare computer simulations of the stochastic Langevin equation for this random diffusion process with analytical results. We explore the regimes of normal Brownian motion as well as anomalous diffusion in the sub- and superdiffusive regimes. We also consider effects of the inertial term on the particle motion. The investigation of the resulting diffusion is performed for unconfined and confined motion.
We investigate the ensemble and time averaged mean squared displacements for particle diffusion in a simple model for disordered media by assuming that the local diffusivity is both fluctuating in time and has a deterministic average growth or decay in time. In this study we compare computer simulations of the stochastic Langevin equation for this random diffusion process with analytical results. We explore the regimes of normal Brownian motion as well as anomalous diffusion in the sub- and superdiffusive regimes. We also consider effects of the inertial term on the particle motion. The investigation of the resulting diffusion is performed for unconfined and confined motion.
We consider the diffusion-advection problem in two simple cellular flow models ( often invoked as examples of subdiffusive tracer motion) and concentrate on the intermediate time range, in which the tracer motion indeed may show subdiffusion. We perform extensive numerical simulations of the systems under different initial conditions and show that the pure intermediate-time subdiffusion regime is only evident when the particles start at the border between different cells, i.e., at the separatrix, and is less pronounced or absent for other initial conditions. The motion moreover shows quite peculiar aging properties, which are also mirrored in the behavior of the time-averaged mean squared displacement for single trajectories. This kind of behavior is due to the complex motion of tracers trapped inside the cell and is absent in classical models based on continuous-time random walks with no dynamics in the trapped state.
A topic of intense current investigation pursues the question of how the highly crowded environment of biological cells affects the dynamic properties of passively diffusing particles. Motivated by recent experiments we report results of extensive simulations of the motion of a finite sized tracer particle in a heterogeneously crowded environment made up of quenched distributions of monodisperse crowders of varying sizes in finite circular two-dimensional domains. For given spatial distributions of monodisperse crowders we demonstrate how anomalous diffusion with strongly non-Gaussian features arises in this model system. We investigate both biologically relevant situations of particles released either at the surface of an inner domain or at the outer boundary, exhibiting distinctly different features of the observed anomalous diffusion for heterogeneous distributions of crowders. Specifically we reveal an asymmetric spreading of tracers even at moderate crowding. In addition to the mean squared displacement (MSD) and local diffusion exponent we investigate the magnitude and the amplitude scatter of the time averaged MSD of individual tracer trajectories, the non-Gaussianity parameter, and the van Hove correlation function. We also quantify how the average tracer diffusivity varies with the position in the domain with a heterogeneous radial distribution of crowders and examine the behaviour of the survival probability and the dynamics of the tracer survival probability. Inter alia, the systems we investigate are related to the passive transport of lipid molecules and proteins in two-dimensional crowded membranes or the motion in colloidal solutions or emulsions in effectively two-dimensional geometries, as well as inside supercrowded, surface adhered cells.
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.
We present the Neural-network-based Upper hybrid Resonance Determination (NURD) algorithm for automatic inference of the electron number density from plasma wave measurements made on board NASA's Van Allen Probes mission. A feedforward neural network is developed to determine the upper hybrid resonance frequency, fuhr, from electric field measurements, which is then used to calculate the electron number density. In previous missions, the plasma resonance bands were manually identified, and there have been few attempts to do robust, routine automated detections. We describe the design and implementation of the algorithm and perform an initial analysis of the resulting electron number density distribution obtained by applying NURD to 2.5 years of data collected with the Electric and Magnetic Field Instrument Suite and Integrated Science (EMFISIS) instrumentation suite of the Van Allen Probes mission. Densities obtained by NURD are compared to those obtained by another recently developed automated technique and also to an existing empirical plasmasphere and trough density model.
We introduce azobenzene-functionalized polyelectrolyte multilayers as efficient, inexpensive optoacoustic transducers for hyper-sound strain waves in the GHz range. By picosecond transient reflectivity measurements we study the creation of nanoscale strain waves, their reflection from interfaces, damping by scattering from nanoparticles and propagation in soft and hard adjacent materials like polymer layers, quartz and mica. The amplitude of the generated strain epsilon similar to 5 x 10(-4) is calibrated by ultrafast X-ray diffraction.
B fields in OB stars (BOB): Detection of a magnetic field in the He-strong star CPD-57 degrees 3509
(2016)
Methods. Spectropolarimetric observations with FORS2 and HARPSpol are analysed using two independent approaches to quantify the magnetic field strength. A high-S/N FLAMES/GIRAFFE spectrum is analysed using a hybrid non-LTE model atmosphere technique. Comparison with stellar evolution models constrains the fundamental parameters of the star. Results. We obtain a firm detection of a surface averaged longitudinal magnetic field with a maximum amplitude of about 1 kG. Assuming a dipolar configuration of the magnetic field, this implies a dipolar field strength larger than 3.3 kG. Moreover, the large amplitude and fast variation (within about 1 day) of the longitudinal magnetic field implies that CPD-57 degrees 3509 is spinning very fast despite its apparently slow projected rotational velocity. The star should be able to support a centrifugal magnetosphere, yet the spectrum shows no sign of magnetically confined material; in particular, emission in H alpha is not observed. Apparently, the wind is either not strong enough for enough material to accumulate in the magnetosphere to become observable or, alternatively, some leakage process leads to loss of material from the magnetosphere. The quantitative spectroscopic analysis of the star yields an effective temperature and a logarithmic surface gravity of 23 750 +/- 250 K and 4.05 +/- 0.10, respectively, and a surface helium fraction of 0.28 +/- 0.02 by number. The surface abundances of C, N, O, Ne, S, and Ar are compatible with the cosmic abundance standard, whereas Mg, Al, Si, and Fe are depleted by about a factor of 2. This abundance pattern can be understood as the consequence of a fractionated stellar wind. CPD-57 degrees 3509 is one of the most evolved He-strong stars known with an independent age constraint due to its cluster membership.
Breaking news from the HST
(2016)
SAO 244567 is a rare example of a star that allows us to witness stellar evolution in real time. Between 1971 and 1990, it changed from a B-type star into the hot central star of the Stingray Nebula. This observed rapid heating has been a mystery for decades, since it is in strong contradiction with the low mass of the star and canonical post-asymptotic giant branch (AGB) evolution. We speculated that SAO 244567 might have suffered from a late thermal pulse (LTP) and obtained new observations with Hubble Space Telescope (HST)/COS to follow the evolution of the surface properties of SAO 244567 and to verify the LTP hypothesis. Our non-LTE spectral analysis reveals that the star cooled significantly since 2002 and that its envelope is now expanding. Therefore, we conclude that SAO 244567 is currently on its way back towards the AGB, which strongly supports the LTP hypothesis. A comparison with state-of-the-art LTP evolutionary calculations shows that these models cannot fully reproduce the evolution of all surface parameters simultaneously, pointing out possible shortcomings of stellar evolution models. Thereby, SAO 244567 keeps on challenging stellar evolution theory and we highly encourage further investigations.
A very general cosmological consideration suggests that, along with galactic dark matter halos, much smaller dark matter structures may exist. These structures are usually called `clumps', and their mass extends to 10−6 M ⊙ or even lower. The clumps should give the main contribution into the signal of dark matter annihilation, provided that they have survived until the present time. Recent observations favor a cored profile for low-mass astrophysical halos. We consider cored clumps and show that they are significantly less firm than the standard NFW ones. In contrast to the standard scenario, the cored clumps should have been completely destroyed inside ~ 20 kpc from the Milky Way center. The dwarf spheroidals should not contain any dark matter clumps. On the other hand, even under the most pessimistic assumption about the clump structure, the clumps should have survived in the Milky Way at a distance exceeding 50 kpc from the center, as well as in low-density cosmic structures. There they significantly boost the dark matter annihilation. We show that at least 70% of the clumps endured the primordial structure formation should still exist untouched in the present-day Universe.
We show systematic electrical impedance measurements of single motile cells on microelectrodes. Wild-type cells and mutant strains were studied that differ in their cell-substrate adhesion strength. We recorded the projected cell area by time-lapse microscopy and observed irregular oscillations of the cell shape. These oscillations were correlated with long-term variations in the impedance signal. Superposed to these long-term trends, we observed fluctuations in the impedance signal. Their magnitude clearly correlated with the adhesion strength, suggesting that strongly adherent cells display more dynamic cell-substrate interactions.
We present a simple setup that exploits the interference of entangled photon pairs. 'Signal' photons are sent through a Mach–Zehnder-like interferometer, while 'idlers' are detected in a variable polarization state. Two-photon interference (in coincidence detection) is observed with very high contrast and for significant time delays between signal and idler detection events. This is explained by quantum erasure of the polarization tag and a delayed choice protocol involving a non-local virtual polarizer. The phase of the two-photon fringes is scanned by varying the path length in the signal beam or by rotating a birefringent crystal in the idler beam. We exploit this to characterize one beam splitter of the signal photon interferometer (reflection and transmission amplitudes including losses), using only information about coincidences and control parameters in the idler path. This is possible because our bi-photon state saturates the Greenberger–Yelin–Englert inequality between contrast and predictability.
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.
Time-delayed collection field experiments are applied to planar organometal halide perovskite (CH3NH3PbI3) based solar cells to investigate charge carrier recombination in a fully working solar cell at the nanosecond to microsecond time scale. Recombination of mobile (extractable) charges is shown to follow second-order recombination dynamics for all fluences and time scales tested. Most importantly, the bimolecular recombination coefficient is found to be time-dependent, with an initial value of ca. 10(-9) cm(3)/s and a progressive reduction within the first tens of nanoseconds. Comparison to the prototypical organic bulk heterojunction device PTB7:PC71BM yields important differences with regard to the mechanism and time scale of free carrier recombination. (C) 2016 AIP Publishing LLC.
Efficient electrical doping of organic semiconductors is a necessary prerequisite for the fabrication of high performance organic electronic devices. In this work, we study p-type doping of poly(3-hexylthiophene) (P3HT) with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F(4)TCNQ) spin-cast from two different solvents. Using electron diffraction, we find strong dopant-induced pi-pi-stacking for films from the solvent chloroform, but not from chlorobenzene. This image is confirmed and expanded by the analysis of vibrational features of P3HT and polaron absorptions using optical spectroscopy. Here, a red-shifted polaron absorption is found in doped films from chloroform, caused by a higher conjugation length of the polymer backbone. These differences result in a higher conductivity of films from chloroform. We use optical spectroscopy on the corresponding blend solutions to shed light on the origin of this effect and propose a model to explain why solutions of doped P3HT reveal more aggregation of charged molecules in chlorobenzene, whereas more order is finally observed in dried films from chloroform. Our study emphasizes the importance of solvent parameters exceeding the bare solubility of pure dopant and host material for the preparation of highly conductive doped films.
Context. Most theoretical investigations of dust charging processes in space have treated the current balance condition as independent of grain size. However, for small grains, since they are often observed in space environments, a dependence on grain size is expected owing to secondary electron emission (SEE). Here, by the term "small" we mean a particle size comparable to the typical penetration depth for given primary electron energy. The results are relevant for the dynamics of small, charged dust particles emitted by the volcanic moon Io, which forms the Jovian dust streams. Aims. We revise the theory of charging of small (submicron sized) micrometeoroids to take into account a high production of secondary electrons for small grains immersed in an isotropic flux of electrons. We apply our model to obtain an improved estimate for the charge of the dust streams leaving the Jovian system, detected by several spacecraft. Methods. We apply a continuum model to describe the penetration of primary electrons in a grain and the emission of secondary electrons along the path. Averaging over an isotropic flux of primaries, we derive a new expression for the secondary electron yield, which can be used to express the secondary electron current on a grain. Results. For the Jupiter plasma environment we derive the surface potential of grains composed of NaCl (believed to be the major constituent of Jovian dust stream particles) or silicates. For small particles, the potential depends on grain size and the secondary electron current induces a sensitivity to material properties. As a result of the small particle effect, the estimates for the charging times and for the fractional charge fluctuations of NaCl grains obtained using our general approach to SEE give results qualitatively different from the analogous estimates derived from the traditional approach to SEE. We find that for the charging environment considered in this paper field emission does not limit the charging of NaCl grains.
The concept of bonding and antibonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Here we apply time-resolved soft X-ray spectroscopy at a free electron laser to directly observe the decreased bonding antibonding splitting following bond-activation using an ultrashort optical laser pulse.
The accretion of the stellar wind material by a compact object represents the main mechanism powering the X-ray emission in classical supergiant high mass X-ray binaries and supergiant fast X-ray transients. In this work we present the first attempt to simulate the accretion process of a fast and dense massive star wind onto a neutron star, taking into account the effects of the centrifugal and magnetic inhibition of accretion ("gating") due to the spin and magnetic field of the compact object. We made use of a radiative hydrodynamical code to model the nonstationary radiatively driven wind of an O-B supergiant star and then place a neutron star characterized by a fixed magnetic field and spin period at a certain distance from the massive companion. Our calculations follow, as a function of time (on a total timescale of several hours), the transitions of the system through all different accretion regimes that are triggered by the intrinsic variations in the density and velocity of the nonstationary wind. The X-ray luminosity released by the system is computed at each time step by taking into account the relevant physical processes occurring in the different accretion regimes. Synthetic lightcurves are derived and qualitatively compared with those observed from classical supergiant high mass X-ray binaries and supergiant fast X-ray transients. Although a number of simplifications are assumed in these calculations, we show that taking into account the effects of the centrifugal and magnetic inhibition of accretion significantly reduces the average X-ray luminosity expected for any neutron star wind-fed binary. The present model calculations suggest that long spin periods and stronger magnetic fields are favored in order to reproduce the peculiar behavior of supergiant fast X-ray transients in the X-ray domain.
Large-scale transitions in societies are associated with both individual behavioural change and restructuring of the social network. These two factors have often been considered independently, yet recent advances in social network research challenge this view. Here we show that common features of societal marginalization and clustering emerge naturally during transitions in a co-evolutionary adaptive network model. This is achieved by explicitly considering the interplay between individual interaction and a dynamic network structure in behavioural selection. We exemplify this mechanism by simulating how smoking behaviour and the network structure get reconfigured by changing social norms. Our results are consistent with empirical findings: The prevalence of smoking was reduced, remaining smokers were preferentially connected among each other and formed increasingly marginalized clusters. We propose that self-amplifying feedbacks between individual behaviour and dynamic restructuring of the network are main drivers of the transition. This generative mechanism for co-evolution of individual behaviour and social network structure may apply to a wide range of examples beyond smoking.
We consider a generalized diffusion equation in two dimensions for modeling diffusion on a comb-like structures. We analyze the probability distribution functions and we derive the mean squared displacement in x and y directions. Different forms of the memory kernels (Dirac delta, power-law, and distributed order) are considered. It is shown that anomalous diffusion may occur along both x and y directions. Ultraslow diffusion and some more general diffusive processes are observed as well. We give the corresponding continuous time random walk model for the considered two dimensional diffusion-like equation on a comb, and we derive the probability distribution functions which subordinate the process governed by this equation to the Wiener process.
We perform experiments and phase model simulations with a ring network of oscillatory electrochemical reactions to explore the effect of random connections and nonisochronicity of the interactions on the pattern formation. A few additional links facilitate the emergence of the fully synchronized state. With larger nonisochronicity, complex rotating waves or persistent irregular phase dynamics can derail the convergence to global synchronization. The observed long transients of irregular phase dynamics exemplify the possibility of a sudden onset of hypersynchronous behavior without any external stimulus or network reorganization.
Consequences of twenty-first-century policy for multi-millennial climate
and sea-level change
(2016)
Most of the policy debate surrounding the actions needed to mitigate and adapt to anthropogenic climate change has been framed by observations of the past 150 years as well as climate and sea-level projections for the twenty-first century. The focus on this 250-year window, however, obscures some of the most profound problems associated with climate change. Here, we argue that the twentieth and twenty-first centuries, a period during which the overwhelming majority of human-caused carbon emissions are likely to occur, need to be placed into a long-term context that includes the past 20 millennia, when the last Ice Age ended and human civilization developed, and the next ten millennia, over which time the projected impacts of anthropogenic climate change will grow and persist. This long-term perspective illustrates that policy decisions made in the next few years to decades will have profound impacts on global climate, ecosystems and human societies - not just for this century, but for the next ten millennia and beyond.
Since more than 15 years, the Cluster mission passes through Earth's radiation belts at least once every 2 days for several hours, measuring the electron intensity at energies from 30 to 400 keV. These data have previously been considered not usable due to contamination caused by penetrating energetic particles (protons at >100 keV and electrons at >400 keV). In this study, we assess the level of distortion of energetic electron spectra from the Research with Adaptive Particle Imaging Detector (RAPID)/Imaging Electron Spectrometer (IES) detector, determining the efficiency of its shielding. We base our assessment on the analysis of experimental data and a radiation transport code (Geant4). In simulations, we use the incident particle energy distribution of the AE9/AP9 radiation belt models. We identify the Roederer L values, L⋆, and energy channels that should be used with caution: at 3≤L⋆≤4, all energy channels (40–400 keV) are contaminated by protons (≃230 to 630 keV and >600 MeV); at L⋆≃1 and 4–6, the energy channels at 95–400 keV are contaminated by high-energy electrons (>400 keV). Comparison of the data with electron and proton observations from RBSP/MagEIS indicates that the subtraction of proton fluxes at energies ≃ 230–630 keV from the IES electron data adequately removes the proton contamination. We demonstrate the usefulness of the corrected data for scientific applications.
We study the adsorption–desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition—demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces—are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye–Hückel approximation is often not feasible and the nonlinear Poisson–Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson–Boltzmann equation is smaller than the Debye–Hückel result, such that the required critical surface charge density for polyelectrolyte adsorption σc increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical–chemical and biophysical systems.
We study the adsorption-desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces-are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye-Huckel approximation is often not feasible and the nonlinear Poisson-Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson-Boltzmann equation is smaller than the Debye-Huckel result, such that the required critical surface charge density for polyelectrolyte adsorption sigma(c) increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical-chemical and biophysical systems.
The past rapid growth of Northern Hemisphere continental ice sheets, which terminated warm and stable climate periods, is generally attributed to reduced summer insolation in boreal latitudes(1-3). Yet such summer insolation is near to its minimum at present(4), and there are no signs of a new ice age(5). This challenges our understanding of the mechanisms driving glacial cycles and our ability to predict the next glacial inception(6). Here we propose a critical functional relationship between boreal summer insolation and global carbon dioxide (CO2) concentration, which explains the beginning of the past eight glacial cycles and might anticipate future periods of glacial inception. Using an ensemble of simulations generated by an Earth system model of intermediate complexity constrained by palaeoclimatic data, we suggest that glacial inception was narrowly missed before the beginning of the Industrial Revolution. The missed inception can be accounted for by the combined effect of relatively high late-Holocene CO2 concentrations and the low orbital eccentricity of the Earth(7). Additionally, our analysis suggests that even in the absence of human perturbations no substantial build-up of ice sheets would occur within the next several thousand years and that the current interglacial would probably last for another 50,000 years. However, moderate anthropogenic cumulative CO2 emissions of 1,000 to 1,500 gigatonnes of carbon will postpone the next glacial inception by at least 100,000 years(8,9). Our simulations demonstrate that under natural conditions alone the Earth system would be expected to remain in the present delicately balanced interglacial climate state, steering clear of both large-scale glaciation of the Northern Hemisphere and its complete deglaciation, for an unusually long time.
We study the damping processes of both incompressible and compressible magnetohydrodynamic (MHD) turbulence in a partially ionized medium. We start from the linear analysis of MHD waves, applying both single-fluid and two-fluid treatments. The damping rates derived from the linear analysis are then used in determining the damping scales of MHD turbulence. The physical connection between the damping scale of MHD turbulence and the cutoff boundary of linear MHD waves is investigated. We find two branches of slow modes propagating in ions and neutrals, respectively, below the damping scale of slow MHD turbulence, and offer a thorough discussion of their propagation and dissipation behavior. Our analytical results are shown to be applicable in a variety of partially ionized interstellar medium (ISM) phases and the solar chromosphere. The importance of neutral viscosity in damping the Alfvenic turbulence in the interstellar warm neutral medium and the solar chromosphere is demonstrated. As a significant astrophysical utility, we introduce damping effects to the propagation of cosmic rays in partially ionized ISM. The important role of turbulence damping in both transit-time damping and gyroresonance is identified.
Even if greenhouse gas emissions were stopped today, sea level would continue to rise for centuries, with the long-term sea-level commitment of a 2 degrees C warmer world significantly exceeding 2 m. In view of the potential implications for coastal populations and ecosystems worldwide, we investigate, from an ice-dynamic perspective, the possibility of delaying sea-level rise by pumping ocean water onto the surface of the Antarctic ice sheet. We find that due to wave propagation ice is discharged much faster back into the ocean than would be expected from a pure advection with surface velocities. The delay time depends strongly on the distance from the coastline at which the additional mass is placed and less strongly on the rate of sea-level rise that is mitigated. A millennium-scale storage of at least 80% of the additional ice requires placing it at a distance of at least 700 km from the coastline. The pumping energy required to elevate the potential energy of ocean water to mitigate the currently observed 3 mmyr(-1) will exceed 7% of the current global primary energy supply. At the same time, the approach offers a comprehensive protection for entire coastlines particularly including regions that cannot be protected by dikes.
Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angstrom spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 angstrom) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.