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Switch It Inside-Out: "Schizophrenic" Behavior of All Thermoresponsive UCST-LCST Diblock Copolymers
(2019)
This feature article reviews our recent advancements on the synthesis, phase behavior, and micellar structures of diblock copolymers consisting of oppositely thermoresponsive blocks in aqueous environments. These copolymers combine a nonionic block, which shows lower critical solution temperature (LCST) behavior, with a zwitterionic block that exhibits an upper critical solution temperature (UCST). The transition temperature of the latter class of polymers is strongly controlled by its molar mass and by the salt concentration, in contrast to the rather invariant transition of nonionic polymers with type II LCST behavior such as poly(N-isopropylacrylamide) or poly(N-isopropyl methacrylamide). This allows for implementing the sequence of the UCST and LCST transitions of the polymers at will by adjusting either molecular or, alternatively, physical parameters. Depending on the location of the transition temperatures of both blocks, different switching scenarios are realized from micelles to inverse micelles, namely via the molecularly dissolved state, the aggregated state, or directly. In addition to studies of (semi)dilute aqueous solutions, highly concentrated systems have also been explored, namely water-swollen thin films. Concerning applications, we discuss the possible use of the diblock copolymers as "smart" nanocarriers.
Spherical particles from shape-memory polymers (SMP) can be stretched to ellipsoids with high aspect ratio (AR) and temporarily stabilized. They can switch back to low AR upon thermal stimulation. Here, the creation of an alternative shape-switching capability of particles from low to high AR is introduced, where a SMP matrix from polyvinyl alcohol (PVA) is used to create crosslinked high AR particles and to program the embedded micrometer-sized particles from a second SMP (oligo(epsilon-caprolactone) micronetworks, MN) with a low switching temperature T-sw. This programming proceeds through shape-recovery of the PVA matrix, from which the MN are harvested by PVA matrix dissolution. The use of a dissolvable SMP matrix may be a general strategy to efficiently create systems with complex moving capabilities.
Binary III-V nitrides such as AlN, GaN and InN in the wurtzite-type structure have long been considered as potent semiconducting materials because of their optoelectronic properties, amongst others. With rising concerns over the utilization of scarce elements, a replacement of the trivalent cations by others in ternary and multinary nitrides has led to the development of different variants of nitrides and oxide nitrides crystallizing in lower-symmetry variants of wurtzite. This work presents the symmetry relationships between these structural types specific to nitrides and oxide nitrides and updates some prior work on this matter. The non-existence of compounds crystallizing in Pmc2(1), formally the highest subgroup of the wurtzite type fulfilling Pauling's rules for 1:1:2 stoichiometries, has been puzzling scientists for a while; a rationalization is given, from a crystallographic basis, of why this space group is unlikely to be adopted.
Networks of coupled dynamical systems provide a powerful way to model systems with enormously complex dynamics, such as the human brain. Control of synchronization in such networked systems has far-reaching applications in many domains, including engineering and medicine. In this paper, we formulate the synchronization control in dynamical systems as an optimization problem and present a multi-objective genetic programming-based approach to infer optimal control functions that drive the system from a synchronized to a non-synchronized state and vice versa. The genetic programming-based controller allows learning optimal control functions in an interpretable symbolic form. The effectiveness of the proposed approach is demonstrated in controlling synchronization in coupled oscillator systems linked in networks of increasing order complexity, ranging from a simple coupled oscillator system to a hierarchical network of coupled oscillators. The results show that the proposed method can learn highly effective and interpretable control functions for such systems.
We investigate synchronization of coupled organ pipes. Synchronization and reflection in the organ lead to undesired weakening of the sound in special cases. Recent experiments have shown that sound interaction is highly complex and nonlinear, however, we show that two delay-coupled Van-der-Pol oscillators appear to be a good model for the occurring dynamical phenomena. Here the coupling is realized as distance-dependent, or time-delayed, equivalently. Analytically, we investigate the synchronization frequency and bifurcation scenarios which occur at the boundaries of the Arnold tongues. We successfully compare our results to experimental data.
Topic and aim. Synchronization in populations of coupled oscillators can be characterized with order parameters that describe collective order in ensembles. A dependence of the order parameter on the coupling constants is well-known for coupled periodic oscillators. The goal of the study is to extend this analysis to ensembles of oscillators with chaotic phases, moreover with phases possessing hyperbolic chaos. Models and methods. Two models are studied in the paper. One is an abstract discrete-time map, composed with a hyperbolic Bernoulli transformation and with Kuramoto dynamics. Another model is a system of coupled continuous-time chaotic oscillators, where each individual oscillator has a hyperbolic attractor of Smale-Williams type. Results. The discrete-time model is studied with the Ott-Antonsen ansatz, which is shown to be invariant under the application of the Bernoulli map. The analysis of the resulting map for the order parameter shows, that the asynchronouis state is always stable, but the synchronous one becomes stable above a certain coupling strength. Numerical analysis of the continuous-time model reveals a complex sequence of transitions from an asynchronous state to a completely synchronous hyperbolic chaos, with intermediate stages that include regimes with periodic in time mean field, as well as with weakly and strongly irregular mean field variations. Discussion. Results demonstrate that synchronization of systems with hyperbolic chaos of phases is possible, although a rather strong coupling is required. The approach can be applied to other systems of interacting units with hyperbolic chaotic dynamics.
We present experimental and numerical evidence of synchronization of burst events in two different modulated CO2 lasers. Bursts appear randomly in each laser as trains of large amplitude spikes intercalated by a small amplitude chaotic regime. Experimental data and model show the frequency locking of bursts in a suitable interval of coupling strength. We explain the mechanism of this phenomenon and demonstrate the inhibitory properties of the implemented coupling.
Synchronization regimes in an ensemble of phase oscillators coupled through a diffusion field
(2022)
We consider an ensemble of identical phase oscillators coupled through a common diffusion field. Using the Ott-Antonsen reduction, we develop dynamical equations for the complex local order parameter and the mean field. The regions of the existence and stability are determined for the totally synchronous, partially synchronous, and asynchronous spatially homogeneous states. A procedure of searching for inhomogeneous states as periodic trajectories of an auxiliary system of the ordinary differential equations is demonstrated. A scenario of emergence of chimera structures from homogeneous synchronous solutions is described.
We consider collective dynamics in the ensemble of serially connected spin-torque oscillators governed by the Landau-Lifshitz-Gilbert-Slonczewski magnetization equation. Proximity to homoclinicity hampers synchronization of spin-torque oscillators: when the synchronous ensemble experiences the homoclinic bifurcation, the growth rate per oscillation of small deviations from the ensemble mean diverges. Depending on the configuration of the contour, sufficiently strong common noise, exemplified by stochastic oscillations of the current through the circuit, may suppress precession of the magnetic field for all oscillators. We derive the explicit expression for the threshold amplitude of noise, enabling this suppression.
For the first time, synchrotron X-ray refraction radiography (SXRR) has been paired with in-situ heat treatment to monitor microstructure and porosity evolution as a function of temperature.
The investigated material was a laser powder bed fusion (LPBF) manufactured AlSi10Mg, where the initial eutectic Si network is known to disintegrate and spherodize into larger particles with increasing temperature.
Such alloy is also prone to ther-mally induced porosity (TIP).
We show that SXRR allows detecting the changes in the Si-phase morphology upon heating, while this is currently possible only using scanning electron microscopy. SXRR also allows observing the growth of pores, usually studied via X-ray computed tomography, but on much smaller fields-of-view.
Our results show the great potential of in-situ SXRR as a tool to gain in-depth knowledge of the susceptibility of any material to thermally induced damage and/or microstructure evolution over statistically relevant volumes.
We propose a simple and eco-friendly method for the formation of composite protein-mineral-microcapsules induced by ultrasound treatment. Protein- and nanoparticle-stabilized oil-in-water (O/W) emulsions loaded with different oils are prepared using high-intensity ultrasound. The formation of thin composite mineral proteinaceous shells is realized with various types of nanoparticles, which are pre-modified with Bovine Serum Albumin (BSA) and subsequently characterized by EDX, TGA, zeta potential measurements and Raman spectroscopy. Cryo-SEM and EDX mapping visualizations show the homogeneous distribution of the densely packed nanoparticles in the capsule shell. In contrast to the results reported in our previous paper,(1) the shell of those nanostructured composite microcapsules is not cross-linked by the intermolecular disulfide bonds between BSA molecules. Instead, a Pickering-Emulsion formation takes place because of the amphiphilicity-driven spontaneous attachment of the BSA-modified nanoparticles at the oil/water interface. Using colloidal particles for the formation of the shell of the microcapsules, in our case silica, hydroxyapatite and calcium carbonate nanoparticles, is promising for the creation of new functional materials. The nanoparticulate building blocks of the composite shell with different chemical, physical or morphological properties can contribute to additional, sometimes even multiple, features of the resulting capsules. Microcapsules with shells of densely packed nanoparticles could find interesting applications in pharmaceutical science, cosmetics or in food technology.
New amphiphilic compounds 1-9 that feature a construction with dendronized hydrophilic and hydrophobic segment groups connected to a specific aromatic or aliphatic spacer unit have been synthesized, following a modular building block strategy. The hydrophilic dendrons are typically branched elements with peripheral carboxylic groups, unlike the hydrophobic dendrons that contain peripheral alkyl chains as part of respective amide functions. The hydrophilic dendrons are in different generations of branching, while the hydrophobic dendrons are all in the first generation of branching (three terminal branching), but differ in the length of the alkyl chains, thus giving rise to designed structure and amphiphilic properties in the new compounds. The resulting surfactants are capable of forming well-defined Langmuir films of remarkable stability when spread from a solution onto an aqueous subphase. Nevertheless, specific packing behaviour and orientation of the amphiphilic molecules were found, depending on the molecular structure, as determined using analysis of the surface pressure-area (pi-A) isotherms. Langmuir-Blodgett transfer of the first monolayer from a pure water subphase to a clean silicon wafer proved possible for the amphiphiles of peripheral alkyl chain length C-12, while the amphiphiles with the longer alkyl chains failed, possibly due to the more rigid monolayers they form, impeding the transfer.
Context. Runaway stars form bow shocks by ploughing through the interstellar medium at supersonic speeds and are promising sources of non-thermal emission of photons. One of these objects has been found to emit non-thermal radiation in the radio band. This triggered the development of theoretical models predicting non-thermal photons from radio up to very-high-energy (VHE, E >= 0.1 TeV) gamma rays. Subsequently, one bow shock was also detected in X-ray observations. However, the data did not allow discrimination between a hot thermal and a non-thermal origin. Further observations of different candidates at X-ray energies showed no evidence for emission at the position of the bow shocks either. A systematic search in the Fermi-LAT energy regime resulted in flux upper limits for 27 candidates listed in the E-BOSS catalogue. Aims. Here we perform the first systematic search for VHE gamma-ray emission from bow shocks of runaway stars. Methods. Using all available archival H.E.S.S. data we search for very-high-energy gamma-ray emission at the positions of bow shock candidates listed in the second E-BOSS catalogue release. Out of the 73 bow shock candidates in this catalogue, 32 have been observed with H.E.S.S. Results. None of the observed 32 bow shock candidates in this population study show significant emission in the H.E.S.S. energy range. Therefore, flux upper limits are calculated in five energy bins and the fraction of the kinetic wind power that is converted into VHE gamma rays is constrained. Conclusions. Emission from stellar bow shocks is not detected in the energy range between 0.14 and 18 TeV. The resulting upper limits constrain the level of VHE gamma-ray emission from these objects down to 0.1-1% of the kinetic wind energy.
Excited-state proton transfer (ESPT) is a fundamental process in biomolecular photochemistry, but its underlying mediators often evade direct observation. We identify a distinct pathway for ESPT in aqueous 2-thiopyridone, by employing transient N1s X-ray absorption spectroscopy and multi-configurational spectrum simulations. Photoexcitations to the singlet S-2 and S-4 states both relax promptly through intersystem crossing to the triplet T-1 state. The T-1 state, through its rapid population and near nanosecond lifetime, mediates nitrogen site deprotonation by ESPT in a secondary intersystem crossing to the S-0 potential energy surface. This conclusively establishes a dominant ESPT pathway for the system in aqueous solution, which is also compatible with previous measurements in acetonitrile. Thereby, the hitherto open questions of the pathway for ESPT in the compound, including its possible dependence on excitation wavelength and choice of solvent, are resolved.
Tautomerism is one of the most important forms of isomerism, owing to the facile interconversion between species and the large differences in chemical properties introduced by the proton transfer connecting the tautomers. Spectroscopic techniques are often used for the characterization of tautomers. In this context, separating the overlapping spectral response of coexisting tautomers is a long-standing challenge in chemistry. Here, we demonstrate that by using resonant inelastic X-ray scattering tuned to the core excited states at the site of proton exchange between tautomers one is able to experimentally disentangle the manifold of valence excited states of each tautomer in a mixture. The technique is applied to the prototypical keto-enol equilibrium of 3-hydroxypyridine in aqueous solution. We detect transitions from the occupied orbitals into the LUMO for each tautomer in solution, which report on intrinsic and hydrogen-bond-induced orbital polarization within the pi and sigma manifolds at the proton-transfer site.
Solvent vapor annealing is as an effective and versatile alternative to thermal annealing to equilibrate and control the assembly of polymer chains in thin films. Here, we present scientific and practical aspects of the solvent vapor annealing method, including the discussion of such factors as non-equilibrium conformational states and chain dynamics in thin films in the presence of solvent. Homopolymer and block copolymer films have been used in model studies to evaluate the robustness and the reproducibility of the solvent vapor processing, as well as to assess polymer-solvent interactions under confinement. Advantages of utilizing a well-controlled solvent vapor environment, including practically interesting regimes of weakly saturated vapor leading to poorly swollen states, are discussed. Special focus is given to dual temperature control over the set-up instrumentation and to the potential of solvo-thermal annealing. The evaluated insights into annealing dynamics derived from the studies on block copolymer films can be applied to improve the processing of thin films of crystalline and conjugated polymers as well as polymer composite in confined geometries.
In ferroelectrets, the piezoelectricity stems from the charges of both polarities trapped on the inner surfaces of the cavities in the material, so that its thermal stability is defined by the stability of the respective charges. In the present work, a template-based lamination technique has been employed to fabricate tubular-channel ferroelectrets from fluoroethylenepropylene (FEP) films. It has been shown that the piezoelectricity in FEP ferroelectrets decays at relatively low temperatures due to the inherently lower thermal stability of the positive charge. In order to improve charge trapping, we have treated both FEP films and inner surfaces of the ferroelectret cavities with titanium-tetrachloride vapor, using the atomic-layer-deposition technique. Using surface-potential-decay measurements on FEP films, we have found that the charge-decay curves shift by more than 100 degrees C to the higher temperatures as a result of the surface treatment. Direct measurements of piezoelectric d(33) coefficients as a function of temperature have shown that the piezoelectric stability is likewise improved with the d(33)-decay curves shifted by 60 degrees C to the right. The improvement of electret/ferroelectret properties can be attributed to the formation of the deeper traps on the chemically modified FEP surface. SEM micrographs and EDS analysis reveal island-like structures with titanium- and oxygen-containing species that can be responsible for the deeper trapping of the electret charges. Published by AIP Publishing.
Context.
The supergiant ionized shell SMC-SGS 1 (DEM 167), which is located in the outer Wing of the Small Magellanic Cloud (SMC), resembles structures that originate from an energetic star-formation event and later stimulate star formation as they expand into the ambient medium. However, stellar populations within and surrounding SMC-SGS 1 tell a different story. Aims. We present a photometric study of the stellar population encompassed by SMC-SGS 1 in order to trace the history of such a large structure and its potential influence on star formation within the low-density, low-metallicity environment of the SMC.
Methods.
For a stellar population that is physically associated with SMC-SGS 1, we combined near-ultraviolet (NUV) photometry from the Galaxy Evolution Explorer with archival optical (V-band) photometry from the ESO Danish 1.54 m Telescope. Given their colors and luminosities, we estimated stellar ages and masses by matching observed photometry to theoretical stellar isochrone models. Results. We find that the investigated region supports an active, extended star-formation event spanning similar to 25-40 Myr ago, as well as continued star formation into the present. Using a standard initial mass function, we infer a lower bound on the stellar mass from this period of similar to 3 x 10(4) M-circle dot, corresponding to a star-formation intensity of similar to 6 x 10(-3) M-circle dot kpc(-2) yr(-1).
Conclusions.
The spatial and temporal distributions of young stars encompassed by SMC-SGS 1 imply a slow, consistent progression of star formation over millions of years. Ongoing star formation, both along the edge and interior to SMC-SGS 1, suggests a combined stimulated and stochastic mode of star formation within the SMC Wing. We note that a slow expansion of the shell within this low-density environment may preserve molecular clouds within the volume of the shell, leaving them to form stars even after nearby stellar feedback expels local gas and dust.
As VLSI design moves into ultra-deep-submicron technologies, timing margins added to the clock period are mandatory, to ensure correct circuit behavior under worst-case conditions. Timing resilient architectures emerged as a promising solution to alleviate these worst-case timing margins. These architectures allow improving system performance and reducing energy consumption. Asynchronous systems, on the other hand, have the potential to improve energy efficiency and performance. Blade is an asynchronous timing resilient template that leverages the advantages of both asynchronous and timing resilient techniques. However, Blade still presents challenges regarding its testability, which hinders its commercial or large-scale application. This paper demonstrates that scan chains can be prohibitive for Blade due to their high silicon costs., which can reach more than 100%. Then, it proposes an alternative test approach that allows concurrent testing, stuck-at, and delay testing. The test approach is based on the reuse the Blade features to provide testability, with silicon area overheads between 4 and 7%.
Both the C-13 chemical shift and the calculated anisotropy effect (spatial magnetic properties) of the electron-deficient centre of stable, crystalline, and structurally characterized carbenes have been employed to unequivocally characterize potential resonance contributors to the present mesomerism (carbene, ylide, betaine, and zwitter ion) and to determine quantitatively the electron deficiency of the corresponding carbene carbon atom. Prior to that, both structures and C-13 chemical shifts were calculated and compared with the experimental delta(C-13)/ppm values and geometry parameters (as a quality criterion for obtained structures).
The blazar Mrk 501 (z = 0.034) was observed at very-high-energy (VHE, E greater than or similar to 100 GeV) gamma-ray wavelengths during a bright flare on the night of 2014 June 23-24 (MJD 56832) with the H.E.S.S. phase-II array of Cherenkov telescopes. Data taken that night by H.E.S.S. at large zenith angle reveal an exceptional number of gamma-ray photons at multi-TeV energies, with rapid flux variability and an energy coverage extending significantly up to 20 TeV. This data set is used to constrain Lorentz invariance violation (LIV) using two independent channels: a temporal approach considers the possibility of an energy dependence in the arrival time of gamma-rays, whereas a spectral approach considers the possibility of modifications to the interaction of VHE gamma-rays with extragalactic background light (EBL) photons. The non-detection of energy-dependent time delays and the non-observation of deviations between the measured spectrum and that of a supposed power-law intrinsic spectrum with standard EBL attenuation are used independently to derive strong constraints on the energy scale of LIV (E-QG) in the subluminal scenario for linear and quadratic perturbations in the dispersion relation of photons. For the case of linear perturbations, the 95% confidence level limits obtained are E-QG,E-1 > 3.6 x 10(17) GeV using the temporal approach and E-QG,E-1 > 2.6 x 10(19) GeV using the spectral approach. For the case of quadratic perturbations, the limits obtained are E-QG,E-2 > 8.5 x 10(10) GeV using the temporal approach and E-QG,E-2 > 7.8 x 10(11) GeV using the spectral approach.
The Sun’s atmosphere is frequently disrupted by coronal mass ejections (CMEs), coupled with flares and energetic particles. The coupling is usually attributed to magnetic reconnection at a vertical current sheet connecting the flare and CME, with the latter embedding a helical magnetic structure known as flux rope. However, both the origin of flux ropes and their nascent paths toward eruption remain elusive. Here, we present an observation of how a stellar-sized CME bubble evolves continuously from plasmoids, mini flux ropes that are barely resolved, within half an hour. The eruption initiates when plasmoids springing from a vertical current sheet merge into a leading plasmoid, which rises at increasing speeds and expands impulsively into the CME bubble, producing hard x-ray bursts simultaneously. This observation illuminates a complete CME evolutionary path capable of accommodating a wide variety of plasma phenomena by bridging the gap between microscale and macroscale dynamics.
The Bow on a String
(2018)
The interaction between a bowed string instrument and its player is conveyed by the bow, the vibrational properties of which can be measured either separately on the bow or during the bowing procedure. Here, two piezoelectric film sensors, made of a ferroelectret material, are installed on a violin bow, one sensor at the tip and one at the frog. With these sensors, a violin is played under normal conditions, and the signals are analysed. The features in the resulting spectrograms are identified as string harmonics and longitudinal bow-hair resonances. The bow-hair sections on both sides of the bow-string contact exhibit separate resonances which are observed as absorption dips in the spectra. Owing to the sensor positions at the bow-hair terminations, it can be inferred that the two bow-hair sections act as mutual vibration absorbers. From a regression of the observed resonances, the longitudinal bow-hair velocity can be obtained. With additional film sensors under the violin bridge, body vibrations were also detected providing further details of the coupling mechanisms.
SwSt 1 (PN G001.5-06.7) is a bright and compact planetary nebula containing a late [WC]-type central star. Previous studies suggested that the nebular and stellar lines are slowly changing with time. We studied new and archival optical and ultraviolet spectra of the object. The [O III] 4959 and 5007 angstrom to H beta line flux ratios decreased between about 1976 and 1997/2015. The stellar spectrum also shows changes between these epochs. We modelled the stellar and nebular spectra observed at different epochs. The analyses indicate a drop of the stellar temperature from about 42 kK to 40.5 kK between 1976 and 1993. We do not detect significant changes between 1993 and 2015. The observations show that the star performed a loop in the H-R diagram. This is possible when a shell source is activated during its post-AGB evolution. We infer that a late thermal pulse (LTP) experienced by a massive post-AGB star can explain the evolution of the central star. Such a star does not expand significantly as the result of the LTP and does not became a born-again red giant. However, the released energy can remove the tiny H envelope of the star.
Porous ceramic diesel particulate filters (DPFs) are extruded products that possess macroscopic anisotropic mechanical and thermal properties. This anisotropy is caused by both morphological features (mostly the orientation of porosity) and crystallographic texture. We systematically studied those two aspects in two aluminum titanate ceramic materials of different porosity using mercury porosimetry, gas adsorption, electron microscopy, X-ray diffraction, and X-ray refraction radiography. We found that a lower porosity content implies a larger isotropy of both the crystal texture and the porosity orientation. We also found that, analogous to cordierite, crystallites do align with their axis of negative thermal expansion along the extrusion direction. However, unlike what found for cordierite, the aluminium titanate crystallite form is such that a more pronounced (0 0 2) texture along the extrusion direction implies porosity aligned perpendicular to it.
Auger-photoelectron coincidence spectroscopy (APECS) has been used to examine the electron correlation and itinerance effects in transition metals Cu, Ni and Co.
It is shown that the LVV Auger, in coincidence with 2p photoelectrons, spectra can be represented using atomic multiplet positions if the 3d-shell is localized (atomic-like) and with a self-convoluted valence band for band-like (itinerant) materials as explained using the Cini-Sawatzky model.
For transition metals, the 3d band changes from band-like to localized with increasing atomic number, with the possibility of a mixed behavior.
Our result shows that the LVV spectra of Cu can be represented by atomic multiplet calculations, those of Co resemble the self-convolution of the valence band and those of Ni are a mixture of both, consistent with the Cini-Sawatzky model.
The stratospheric polar vortex can influence the tropospheric circulation and thereby winter weather in the mid-latitudes. Weak vortex states, often associated with sudden stratospheric warmings (SSW), have been shown to increase the risk of cold-spells especially over Eurasia, but its role for North American winters is less clear. Using cluster analysis, we show that there are two dominant patterns of increased polar cap heights in the lower stratosphere. Both patterns represent a weak polar vortex but they are associated with different wave mechanisms and different regional tropospheric impacts. The first pattern is zonally symmetric and associated with absorbed upward-propagating wave activity, leading to a negative phase of the North Atlantic Oscillation (NAO) and cold-air outbreaks over northern Eurasia. This coupling mechanism is well-documented in the literature and is consistent with the downward migration of the northern annular mode (NAM). The second pattern is zonally asymmetric and linked to downward reflected planetary waves over Canada followed by a negative phase of the Western Pacific Oscillation (WPO) and cold-spells in Central Canada and the Great Lakes region. Causal effect network (CEN) analyses confirm the atmospheric pathways associated with this asymmetric pattern. Moreover, our findings suggest the reflective mechanism to be sensitive to the exact region of upward wave-activity fluxes and to be state-dependent on the strength of the vortex. Identifying the causal pathways that operate on weekly to monthly timescales can pave the way for improved sub-seasonal to seasonal forecasting of cold spells in the mid-latitudes.
In this study we investigate, using all-atom molecular-dynamics computer simulations, the in-plane diffusion of a doxorubicin drug molecule in a thin film of water confined between two silica surfaces. We find that the molecule diffuses along the channel in the manner of a Gaussian diffusion process, but with parameters that vary according to its varying transversal position. Our analysis identifies that four Gaussians, each describing particle motion in a given transversal region, are needed to adequately describe the data. Each of these processes by itself evolves with time at a rate slower than that associated with classical Brownian motion due to a predominance of anticorrelated displacements. Long adsorption events lead to ageing, a property observed when the diffusion is intermittently hindered for periods of time with an average duration which is theoretically infinite. This study presents a simple system in which many interesting features of anomalous diffusion can be explored. It exposes the complexity of diffusion in nanoconfinement and highlights the need to develop new understanding.
Here, we present novel equations for the large-scale zonal-mean wind as well as those for planetary waves. Together with synoptic parameterization (as presented by Coumou et al., 2011), these form the mathematical description of the dynamical core of Aeolus 1.0. The regions of high azonal wind velocities (planetary waves) are accurately captured for all validation experiments. The zonal-mean zonal wind and the integrated lower troposphere mass flux show good results in particular in the Northern Hemisphere. In the Southern Hemisphere, the model tends to produce too-weak zonal-mean zonal winds and a too-narrow Hadley circulation. We discuss possible reasons for these model biases as well as planned future model improvements and applications.
Both climate-change damages and climate-change mitigation will incur economic costs. While the risk of severe damages increases with the level of global warming (Dell et al., 2014; IPCC, 2014b, 2018; Lenton et al., 2008), mitigating costs increase steeply with more stringent warming limits (IPCC, 2014a; Luderer et al., 2013; Rogelj et al., 2015). Here, we show that the global warming limit that minimizes this century's total economic costs of climate change lies between 1.9 and 2 ∘C, if temperature changes continue to impact national economic growth rates as observed in the past and if instantaneous growth effects are neither compensated nor amplified by additional growth effects in the following years. The result is robust across a wide range of normative assumptions on the valuation of future welfare and inequality aversion. We combine estimates of climate-change impacts on economic growth for 186 countries (applying an empirical damage function from Burke et al., 2015) with mitigation costs derived from a state-of-the-art energy–economy–climate model with a wide range of highly resolved mitigation options (Kriegler et al., 2017; Luderer et al., 2013, 2015). Our purely economic assessment, even though it omits non-market damages, provides support for the international Paris Agreement on climate change. The political goal of limiting global warming to “well below 2 degrees” is thus also an economically optimal goal given above assumptions on adaptation and damage persistence.
Macro-economic assessments of climate impacts lack an analysis of the distribution of daily rainfall, which can resolve both complex societal impact channels and anthropogenically forced changes(1-6). Here, using a global panel of subnational economic output for 1,554 regions worldwide over the past 40 years, we show that economic growth rates are reduced by increases in the number of wet days and in extreme daily rainfall, in addition to responding nonlinearly to the total annual and to the standardized monthly deviations of rainfall. Furthermore, high-income nations and the services and manufacturing sectors are most strongly hindered by both measures of daily rainfall, complementing previous work that emphasized the beneficial effects of additional total annual rainfall in low-income, agriculturally dependent economies(4,7). By assessing the distribution of rainfall at multiple timescales and the effects on different sectors, we uncover channels through which climatic conditions can affect the economy. These results suggest that anthropogenic intensification of daily rainfall extremes(8-10) will have negative global economic consequences that require further assessment by those who wish to evaluate the costs of anthropogenic climate change.
The diffusion in the comb structures is a popular model of geometrically induced anomalous diffusion. In the present work we concentrate on the diffusion along the backbone in a system where sidebranches are planes, and the diffusion thereon is anomalous and described by continuous time random walks (CTRW). We show that the mean squared displacement (MSD) in the backbone of the comb behaves differently depending on whether the waiting time periods in the sidebranches are reset after the step in the backbone is done (a rejuvenating junction model), or not (a non-rejuvenating junction model). In the rejuvenating case the subdiffusion in the sidebranches only changes the prefactor in the ultra-slow (logarithmic) diffusion along the backbone, while in the non-rejuvenating case the ultraslow, logarithmic subdiffusion is changed to a much faster power-law subdiffusion (with a logarithmic correction) as it was found earlier by Iomin and Mendez [25]. Moreover, in the first case the result does not change if the diffusion in the backbone is itself anomalous, while in the second case it does. Two of the special cases of the considered models (the non-rejuvenating junction under normal diffusion in the backbone, and rejuvenating junction for the same waiting time distribution in the sidebranches and in junction points) were also investigated within the approach based on the corresponding generalized Fokker-Planck equations. (c) 2017 Elsevier Ltd. All rights reserved.
This work revisits the electrostatic instability for blazar-induced pair beams propagating through the intergalactic medium (IGM) using linear analysis and PIC simulations. We study the impact of the realistic distribution function of pairs resulting from the interaction of high-energy gamma-rays with the extragalactic background light. We present analytical and numerical calculations of the linear growth rate of the instability for the arbitrary orientation of wave vectors. Our results explicitly demonstrate that the finite angular spread of the beam dramatically affects the growth rate of the waves, leading to the fastest growth for wave vectors quasi-parallel to the beam direction and a growth rate at oblique directions that is only a factor of 2-4 smaller compared to the maximum. To study the nonlinear beam relaxation, we performed PIC simulations that take into account a realistic wide-energy distribution of beam particles. The parameters of the simulated beam-plasma system provide an adequate physical picture that can be extrapolated to realistic blazar-induced pairs. In our simulations, the beam looses only 1% of its energy, and we analytically estimate that the beam would lose its total energy over about 100 simulation times. An analytical scaling is then used to extrapolate the parameters of realistic blazar-induced pair beams. We find that they can dissipate their energy slightly faster by the electrostatic instability than through inverse-Compton scattering. The uncertainties arising from, e.g., details of the primary gamma-ray spectrum are too large to make firm statements for individual blazars, and an analysis based on their specific properties is required.
We present a survey for metal absorption systems traced by neutral oxygen over 3.2 < z < 6.5. Our survey uses Keck/ESI and VLT/X-Shooter spectra of 199 QSOs with redshifts up to 6.6. In total, we detect 74 OI absorbers, of which 57 are separated from the background QSO by more than 5000 km s(-1). We use a maximum likelihood approach to fit the distribution of OI lambda 1302 equivalent widths in bins of redshift and from this determine the evolution in number density of absorbers with W-1302 > 0.05 angstrom, of which there are 49 nonproximate systems in our sample. We find that the number density does not monotonically increase with decreasing redshift, as would naively be expected from the buildup of metal-enriched circumgalactic gas with time. The number density over 4.9 < z < 5.7 is a factor of 1.7-4.1 lower (68% confidence) than that over 5.7 < z < 6.5, with a lower value at z < 5.7 favored with 99% confidence. This decrease suggests that the fraction of metals in a low-ionization phase is larger at z similar to 6 than at lower redshifts. Absorption from highly ionized metals traced by CIV is also weaker in higher-redshift OI systems, supporting this picture. The evolution of OI absorbers implies that metal-enriched circumgalactic gas at z similar to 6 is undergoing an ionization transition driven by a strengthening ultraviolet background. This in turn suggests that the reionization of the diffuse intergalactic medium may still be ongoing at or only recently ended by this epoch.
Context. HD 93129A was classified as the earliest O-type star in the Galaxy (O2 If*) and is considered as the prototype of its spectral class. However, interferometry shows that this object is a binary system, while recent observations even suggest a triple configuration. None of the previous spectral analyses of this object accounted for its multiplicity. With new high-resolution UV and optical spectra, we have the possibility to reanalyze this key object, taking its binary nature into account for the first time. Aims. We aim to derive the fundamental parameters and the evolutionary status of HD 93129A, identifying the contributions of both components to the composite spectrum Results. Despite the similar spectral types of the two components, we are able to find signatures from each of the components in the combined spectrum, which allows us to estimate the parameters of both stars. We derive log(L/L-circle dot) = 6.15, T-eff = 52 kK, and log (M)over dot = -4.7[M-circle dot yr(-1)] for the primary Aa, and log(L/L-circle dot) = 5.58, T-eff = 45 kK, and log (M)over dot = -5.8 [M(circle dot)yr(-1)] for the secondary Ab. Conclusions. Even when accounting for the binary nature, the primary of HD 93129A is found to be one of the hottest and most luminous O stars in our Galaxy. Based on the theoretical decomposition of the spectra, we assign spectral types O2 If* and O3 III(f*) to components Aa and Ab, respectively. While we achieve a good fit for a wide spectral range, specific spectral features are not fully reproduced. The data are not sufficient to identify contributions from a hypothetical third component in the system.
Floating ice shelves, which fringe most of Antarctica’s coastline, regulate ice flow into the Southern Ocean1,2,3. Their thinning4,5,6,7 or disintegration8,9 can cause upstream acceleration of grounded ice and raise global sea levels. So far the effect has not been quantified in a comprehensive and spatially explicit manner. Here, using a finite-element model, we diagnose the immediate, continent-wide flux response to different spatial patterns of ice-shelf mass loss. We show that highly localized ice-shelf thinning can reach across the entire shelf and accelerate ice flow in regions far from the initial perturbation. As an example, this ‘tele-buttressing’ enhances outflow from Bindschadler Ice Stream in response to thinning near Ross Island more than 900 km away. We further find that the integrated flux response across all grounding lines is highly dependent on the location of imposed changes: the strongest response is caused not only near ice streams and ice rises, but also by thinning, for instance, well-within the Filchner–Ronne and Ross Ice Shelves. The most critical regions in all major ice shelves are often located in regions easily accessible to the intrusion of warm ocean waters10,11,12, stressing Antarctica’s vulnerability to changes in its surrounding ocean.
Context. Very massive stars pass through the Wolf-Rayet (WR) stage before they finally explode. Details of their evolution have not yet been safely established, and their physics are not well understood. Their spectral analysis requires adequate model atmospheres, which have been developed step by step during the past decades and account in their recent version for line blanketing by the millions of lines from iron and iron-group elements. However, only very few WN stars have been re-analyzed by means of line-blanketed models yet. Aims. The quantitative spectral analysis of a large sample of Galactic WN stars with the most advanced generation of model atmospheres should provide an empirical basis for various studies about the origin, evolution, and physics of the Wolf-Rayet stars and their powerful winds. Methods. We analyze a large sample of Galactic WN stars by means of the Potsdam Wolf-Rayet (PoWR) model atmospheres, which account for iron line blanketing and clumping. The results are compared with a synthetic population, generated from the Geneva tracks for massive star evolution. Results. We obtain a homogeneous set of stellar and atmospheric parameters for the GalacticWN stars, partly revising earlier results. Conclusions. Comparing the results of our spectral analyses of the Galactic WN stars with the predictions of the Geneva evolutionary calculations, we conclude that there is rough qualitative agreement. However, the quantitative discrepancies are still severe, and there is no preference for the tracks that account for the effects of rotation. It seems that the evolution of massive stars is still not satisfactorily understood.
We present the results of the most comprehensive survey of the Galactic plane in very high-energy (VHE) gamma-rays, including a public release of Galactic sky maps, a catalog of VHE sources, and the discovery of 16 new sources of VHE gamma-rays. The High Energy Spectroscopic System (H.E.S.S.) Galactic plane survey (HGPS) was a decade-long observation program carried out by the H.E.S.S. I array of Cherenkov telescopes in Namibia from 2004 to 2013. The observations amount to nearly 2700 h of quality-selected data, covering the Galactic plane at longitudes from l = 250 degrees to 65 degrees and latitudes vertical bar b vertical bar <= 3 degrees. In addition to the unprecedented spatial coverage, the HGPS also features a relatively high angular resolution (0.08 degrees approximate to 5 arcmin mean point spread function 68% containment radius), sensitivity (less than or similar to 1.5% Crab flux for point-like sources), and energy range (0.2-100 TeV). We constructed a catalog of VHE gamma-ray sources from the HGPS data set with a systematic procedure for both source detection and characterization of morphology and spectrum. We present this likelihood-based method in detail, including the introduction of a model component to account for unresolved, large-scale emission along the Galactic plane. In total, the resulting HGPS catalog contains 78 VHE sources, of which 14 are not reanalyzed here, for example, due to their complex morphology, namely shell-like sources and the Galactic center region. Where possible, we provide a firm identification of the VHE source or plausible associations with sources in other astronomical catalogs. We also studied the characteristics of the VHE sources with source parameter distributions. 16 new sources were previously unknown or unpublished, and we individually discuss their identifications or possible associations. We firmly identified 31 sources as pulsar wind nebulae (PWNe), supernova remnants (SNRs), composite SNRs, or gamma-ray binaries. Among the 47 sources not yet identified, most of them (36) have possible associations with cataloged objects, notably PWNe and energetic pulsars that could power VHE PWNe.
More than half of Earth's freshwater resources are held by the Antarctic Ice Sheet, which thus represents by far the largest potential source for global sea-level rise under future warming conditions(1). Its long-term stability determines the fate of our coastal cities and cultural heritage. Feedbacks between ice, atmosphere, ocean, and the solid Earth give rise to potential nonlinearities in its response to temperature changes. So far, we are lacking a comprehensive stability analysis of the Antarctic Ice Sheet for different amounts of global warming. Here we show that the Antarctic Ice Sheet exhibits a multitude of temperature thresholds beyond which ice loss is irreversible. Consistent with palaeodata(2)we find, using the Parallel Ice Sheet Model(3-5), that at global warming levels around 2 degrees Celsius above pre-industrial levels, West Antarctica is committed to long-term partial collapse owing to the marine ice-sheet instability. Between 6 and 9 degrees of warming above pre-industrial levels, the loss of more than 70 per cent of the present-day ice volume is triggered, mainly caused by the surface elevation feedback. At more than 10 degrees of warming above pre-industrial levels, Antarctica is committed to become virtually ice-free. The ice sheet's temperature sensitivity is 1.3 metres of sea-level equivalent per degree of warming up to 2 degrees above pre-industrial levels, almost doubling to 2.4 metres per degree of warming between 2 and 6 degrees and increasing to about 10 metres per degree of warming between 6 and 9 degrees. Each of these thresholds gives rise to hysteresis behaviour: that is, the currently observed ice-sheet configuration is not regained even if temperatures are reversed to present-day levels. In particular, the West Antarctic Ice Sheet does not regrow to its modern extent until temperatures are at least one degree Celsius lower than pre-industrial levels. Our results show that if the Paris Agreement is not met, Antarctica's long-term sea-level contribution will dramatically increase and exceed that of all other sources. <br /> Modelling shows that the Antarctic Ice Sheet exhibits multiple temperature thresholds beyond which ice loss would become irreversible, and once melted, the ice sheet can regain its previous mass only if the climate cools well below pre-industrial temperatures.
Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V-OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V-OC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V-OC of the device. Importantly, the V-OC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the V-OC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the V-OC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces.
Spectroscopic observations play essential roles in astrophysics. They are crucial for determining physical parameters in our Universe, providing information about the chemistry of various astronomical environments. The proper execution of the spectroscopic analysis requires accounting for all the physical effects that are compatible to the signal-to-noise ratio. We find in this paper the influence on spectroscopy from the atomic/ground state alignment owing to anisotropic radiation and modulated by interstellar magnetic field, has significant impact on the study of interstellar gas. In different observational scenarios, we comprehensively demonstrate how atomic alignment influences the spectral analysis and provide the expressions for correcting the effect. The variations are even more pronounced for multiplets and line ratios. We show the variation of the deduced physical parameters caused by the atomic alignment effect, including alpha-to-iron ratio ([X/Fe]) and ionization fraction. Synthetic observations are performed to illustrate the visibility of such effect with current facilities. A study of Photodissociation regions in rho Ophiuchi cloud is presented to demonstrate how to account for atomic alignment in practice. Our work has shown that due to its potential impact, atomic alignment has to be included in an accurate spectroscopic analysis of the interstellar gas with current observational capability.
Bipolar electrets from polypropylene (PP) are essential, e.g., in electret air filters and in cellular-foam ferroelectrets. Therefore, the mechanism of surface-charge stability enhancement on PP electrets via orthophosphoric-acid surface treatment is investigated in detail. It is shown that the significant charge-stability enhancement can be mainly attributed to deeper surface traps originating from deposited chemicals and topographic features on the modified surfaces. Thermally stimulated discharge of chemically treated and non-treated PP films with different surface-charge densities is used to test the limits of the newly formed deep traps in terms of the capacity for hosting surface charges. When the initial surface-charge density is very high, more charges are forced into shallower original traps on the surface or in the bulk of the treated PP samples, reducing the effect of the deeper surface traps brought by the surface modification. The well-known crossover phenomenon (of the surface-charge decay curves) has been observed between modified PP electrets charged to +/- 2kV and to +/- 3kV. Acoustically probed charge distributions in the thickness direction of PP electrets at different stages of thermal discharging indicate that the deep surface trapping sites may have preference for negative charges, resulting in the observed asymmetric charge stability of the modified PP films.
The Influence of the Support Structure on Residual Stress and Distortion in SLM Inconel 718 Parts
(2018)
The effect of support structure and of removal from the base plate on the residual stress state in selective laser melted IN718 parts was studied by means of synchrotron X-ray diffraction. The residual stresses in subsurface region of two elongated prisms in as-built condition and after removal from the base plate were determined. One sample was directly built on a base plate and another one on a support structure. Also, the distortion on the top surface due to stress release was measured by contact profilometry. High tensile residual stress values were found, with pronounced stress gradient along the hatching direction. In the sample on support, stress redistribution took place after removal from the base plate, as opposed to simple stress relaxation for the sample without support. The sample on support structure showed larger distortion compared to sample without support. We conclude that the use of a support decreases stress values but stress-relieving heat treatments are still needed.
Pump-probe photoelectron spectroscopy (PES) is a versatile tool to investigate the dynamics of transient states of excited matter. Vacuum space-charge effects can mask these dynamics and complicate the interpretation of electron spectra. Here we report on space-charge effects in Au 4f photoemission from a polycrystalline gold surface, excited with moderately intense 90 ps (FWHM) soft x-ray probe pulses, under the influence of the Coulomb forces exerted by a pump electron cloud, which was produced by intense 40 fs laser pulses. The experimentally observed kinetic energy shift and spectral broadening of the Au 4f lines, measured with highly-efficient time-of-flight spectroscopy, are in good agreement with simulations utilizing a mean-field model of the electrostatic pump electron potential. This confirms that the line broadening is predominantly caused by variations in the take-off time of the probe electrons without appreciable influence of local scattering events. Our findings might be of general interest for pump-probe PES with picosecond-pulse-length sources.
High diffusion-sensitizing magnetic field gradients have been more and more often applied nowadays to achieve a better characterization of the microstructure. As the resulting spin-echo signal significantly deviates from the conventional Gaussian form, various models have been employed to interpret these deviations and to relate them with the microstructural properties of a sample. In this paper, we argue that the non-Gaussian behavior of the signal is a generic universal feature of the Bloch-Torrey equation. We provide a simple yet rigorous description of the localization regime emerging at high extended gradients and identify its origin as a symmetry breaking at the reflecting boundary. We compare the consequent non-Gaussian signal decay to other diffusion NMR regimes such as slow-diffusion, motional-narrowing and diffusion-diffraction regimes. We emphasize limitations of conventional perturbative techniques and advocate for non-perturbative approaches which may pave a way to new imaging modalities in this field.
We present new calculations of the mass inflow and outflow rates around the Milky Way (MW), derived from a catalog of ultraviolet metal-line high-velocity clouds (HVCs). These calculations are conducted by transforming the HVC velocities into the Galactic standard of rest (GSR) reference frame, identifying inflowing (vGSR.<.0 km s(-1)) and outflowing (vGSR > 0 km s(-1)) populations, and using observational constraints on the distance, metallicity, dust content, covering fractions, and total silicon column density of each population. After removing HVCs associated with the Magellanic Stream and the Fermi Bubbles, we find inflow and outflow rates in cool (T similar to 10(4) K) ionized gas of dM(in)/dt greater than or similar to.(0.53 +/- 0.23)(d/12 kpc)(Z/0.2Z(circle dot))-1M(circle dot) yr(-1) and dM(out)/dt greater than or similar to (0.16 +/- 0.07)(d/12 kpc)(Z/0.5Z(circle dot))M--1(circle dot) yr(-1). The apparent excess of inflowing over outflowing gas suggests that the MW is currently in an inflow-dominated phase, but the presence of substantial mass flux in both directions supports a Galactic fountain model, in which gas is constantly recycled between the disk and the halo. We also find that the metal flux in both directions (in and out) is indistinguishable. By comparing the outflow rate to the Galactic star formation rate, we present the first estimate of the mass loading factor (eta(HVC)) of the disk-wide MW wind, finding eta(HVC) greater than or similar to (0.10 +/- 0.06)(d/12 kpc)(Z/0.5Z(circle dot))(-1). Including the contributions from low- and intermediatevelocity clouds and from hot gas would increase these inflow and outflow estimates.
Understanding and controlling properties of transition metal complexes is a crucial step towards tailoring materials for sustainable energy applications. In a systematic approach, we use resonant inelastic X-ray scattering to study the influence of ligand substitution on the valence electronic structure around an aqueous iron(II) center. Exchanging cyanide with 2-2′-bipyridine ligands reshapes frontier orbitals in a way that reduces metal 3d charge delocalization onto the ligands. This net decrease of metal–ligand covalency results in lower metal-centered excited state energies in agreement with previously reported excited state dynamics. Furthermore, traces of solvent-effects were found indicating a varying interaction strength of the solvent with ligands of different character. Our results demonstrate how ligand exchange can be exploited to shape frontier orbitals of transition metal complexes in solution-phase chemistry; insights upon which future efforts can built when tailoring the functionality of photoactive systems for light-harvesting applications.
The optical signatures of molecular-doping induced polarons in poly(3-hexylthiophene-2,5-diyl)
(2020)
Optical absorption spectroscopy is a key method to investigate doped conjugated polymers and to characterize the doping-induced charge carriers, i.e., polarons. For prototypical poly(3-hexylthiophene-2,5-diyl) (P3HT), the absorption intensity of molecular dopant induced polarons is widely used to estimate the carrier density and the doping efficiency, i.e., the number of polarons formed per dopant molecule. However, the dependence of the polaron-related absorption features on the structure of doped P3HT, being either aggregates or separated individual chains, is not comprehensively understood in contrast to the optical absorption features of neutral P3HT. In this work, we unambiguously differentiate the optical signatures of polarons on individual P3HT chains and aggregates in solution, notably the latter exhibiting the same shape as aggregates in solid thin films. This is enabled by employing tris(pentafluorophenyl)borane (BCF) as dopant, as this dopant forms only ion pairs with P3HT and no charge transfer complexes, and BCF and its anion have no absorption in the spectral region of P3HT polarons. Polarons on individual chains exhibit absorption peaks at 1.5 eV and 0.6 eV, whereas in aggregates the high-energy peak is split into a doublet 1.3 eV and 1.65 eV, and the low-energy peak is shifted below 0.5 eV. The dependence of the fraction of solvated individual chains versus aggregates on absolute solution concentration, dopant concentration, and temperature is elucidated, and we find that aggregates predominate in solution under commonly used processing conditions. Aggregates in BCF-doped P3HT solution can be effectively removed upon simple filtering. From varying the filter pore size (down to 200 nm) and thin film morphology characterization with scanning force microscopy we reveal the aggregates' size dependence on solution absolute concentration and dopant concentration. Furthermore, X-ray photoelectron spectroscopy shows that the dopant loading in aggregates is higher than for individual P3HT chains. The results of this study help understanding the impact of solution pre-aggregation on thin film properties of molecularly doped P3HT, and highlight the importance of considering such aggregation for other doped conjugated polymers in general.
The photon
(2019)
We investigate the role of the spatial mode function in a single-photon experiment designed to demonstrate the principle of complementarity. Our approach employs entangled photons created by spontaneous parametric downconversion from a pump mode in a TEM01 mode together with a double slit. Measuring the interference of the signal photons behind the double slit in coincidence with the entangled idler photons at different positions, we select signal photons of different mode functions. When the signal photons belong to the TEM01-like double-hump mode, we obtain almost perfect visibility of the interference fringes, and no "which slit" information is available in the idler photon detected before the slits. This result is remarkable because the entangled signal and idler photon pairs are created each time in only one of the two intensity humps. However, when we break the symmetry between the two maxima of the signal photon mode structure, the paths through the slits for these additional photons become distinguishable and the visibility vanishes. It is the mode function of the photons selected by the detection system that decides if interference or "which slit" information is accessible in the experiment.
Galactic winds exhibit a multiphase structure that consists of hot-diffuse and cold-dense phases. Here we present high-resolution idealized simulations of the interaction of a hot supersonic wind with a cold cloud with the moving-mesh code AREPO in setups with and without radiative cooling. We demonstrate that cooling causes clouds with sizes larger than the cooling length to fragment in 2D and 3D simulations. We confirm earlier 2D simulations by McCourt et al. (2018) and highlight differences of the shattering processes of 3D clouds that are exposed to a hot wind. The fragmentation process is quantified with a friends-of-friends analysis of shattered cloudlets and density power spectra. Those show that radiative cooling causes the power spectral index to gradually increase when the initial cloud radius is larger than the cooling length and with increasing time until the cloud is fully dissolved in the hot wind. A resolution of around 1 pc is required to reveal the effect of cooling-induced fragmentation of a 100 pc outflowing cloud. Thus, state-of-the-art cosmological zoom simulations of the circumgalactic medium fall short by orders of magnitudes from resolving this fragmentation process. This physics is, however, necessary to reliably model observed column densities and covering fractions of Lyman alpha haloes, high-velocity clouds, and broad-line regions of active galactic nuclei.
Based on data from the ESA Gaia Data Release 2 (DR2) and several ground-based, multi-band photometry surveys we have compiled an all-sky catalogue of 39 800 hot subluminous star candidates selected in Gaia DR2 by means of colour, absolute magnitude, and reduced proper motion cuts. We expect the majority of the candidates to be hot subdwarf stars of spectral type B and O, followed by blue horizontal branch stars of late B-type (HBB), hot post-AGB stars, and central stars of planetary nebulae. The contamination by cooler stars should be about 10%. The catalogue is magnitude limited to Gaia G < 19 mag and covers the whole sky. Except within the Galactic plane and LMC/SMC regions, we expect the catalogue to be almost complete up to about 1.5 kpc. The main purpose of this catalogue is to serve as input target list for the large-scale photometric and spectroscopic surveys which are ongoing or scheduled to start in the coming years. In the long run, securing a statistically significant sample of spectroscopically confirmed hot subluminous stars is key to advance towards a more detailed understanding of the latest stages of stellar evolution for single and binary stars.
The nine-year H.E.S.S. Galactic Plane Survey (HGPS) has yielded the most uniform observation scan of the inner Milky Way in the TeV gamma-ray band to date. The sky maps and source catalogue of the HGPS allow for a systematic study of the population of TeV pulsar wind nebulae found throughout the last decade. To investigate the nature and evolution of pulsar wind nebulae, for the first time we also present several upper limits for regions around pulsars without a detected TeV wind nebula. Our data exhibit a correlation of TeV surface brightness with pulsar spindown power (E) over dot. This seems to be caused both by an increase of extension with decreasing (E) over dot, and hence with time, compatible with a power law R-PWN((E) over dot) similar to(E) over dot(0.65 +/- 0.20), and by a mild decrease of TeV gamma-ray luminosity with decreasing (E) over dot, compatible with L-1 (10 TeV) similar to (E) over dot(0.59 +/- 0.21). We also find that the off sets of pulsars with respect to the wind nebula centre with ages around 10 kyr are frequently larger than can be plausibly explained by pulsar proper motion and could be due to an asymmetric environment. In the present data, it seems that a large pulsar off set is correlated with a high apparent TeV efficiency L1- 10 TeV / (E) over dot. In addition to 14 HGPS sources considered firmly identified pulsar wind nebulae and 5 additional pulsar wind nebulae taken from literature, we find 10 HGPS sources that are likely TeV pulsar wind nebula candidates. Using a model that subsumes the present common understanding of the very high-energy radiative evolution of pulsar wind nebulae, we find that the trends and variations of the TeV observables and limits can be reproduced to a good level, drawing a consistent picture of present-day TeV data and theory.
In this work, we investigate the potassium excess absorption around 7699 Å of the exoplanets HD189733b and HD209458b. For this purpose, we used high-spectral resolution transit observations acquired with the 2 × 8.4 m Large Binocular Telescope (LBT) and the Potsdam Echelle Polarimetric and Spectroscopic Instrument (PEPSI). For a bandwidth of 0.8 Å, we present a detection >7σ with an absorption level of 0.18 per cent for HD189733b. Applying the same analysis to HD209458b, we can set 3σ upper limit of 0.09 per cent, even though we do not detect a K-excess absorption. The investigation suggests that the K feature is less present in the atmosphere of HD209458b than in the one of HD189733b. This comparison confirms previous claims that the atmospheres of these two planets must have fundamentally different properties.
2D Ruddlesden-Popper perovskite (RPP) solar cells have excellent environmental stability. However, the power conversion efficiency (PCE) of RPP cells remains inferior to 3D perovskite-based cells. Herein, 2D (CH3(CH2)(3)NH3)(2)(CH3NH3)(n-1)PbnI3n+1 perovskite cells with different numbers of [PbI6](4-) sheets (n = 2-4) are analyzed. Photoluminescence quantum yield (PLQY) measurements show that nonradiative open-circuit voltage (V-OC) losses outweigh radiative losses in materials with n > 2. The n = 3 and n = 4 films exhibit a higher PLQY than the standard 3D methylammonium lead iodide perovskite although this is accompanied by increased interfacial recombination at the top perovskite/C-60 interface. This tradeoff results in a similar PLQY in all devices, including the n = 2 system where the perovskite bulk dominates the recombination properties of the cell. In most cases the quasi-Fermi level splitting matches the device V-OC within 20 meV, which indicates minimal recombination losses at the metal contacts. The results show that poor charge transport rather than exciton dissociation is the primary reason for the reduction in fill factor of the RPP devices. Optimized n = 4 RPP solar cells had PCEs of 13% with significant potential for further improvements.
Mass loss from the Antarctic Ice Sheet constitutes the largest uncertainty in projections of future sea level rise. Ocean-driven melting underneath the floating ice shelves and subsequent acceleration of the inland ice streams are the major reasons for currently observed mass loss from Antarctica and are expected to become more important in the future. Here we show that for projections of future mass loss from the Antarctic Ice Sheet, it is essential (1) to better constrain the sensitivity of sub-shelf melt rates to ocean warming and (2) to include the historic trajectory of the ice sheet. In particular, we find that while the ice sheet response in simulations using the Parallel Ice Sheet Model is comparable to the median response of models in three Antarctic Ice Sheet Intercomparison projects - initMIP, LARMIP-2 and ISMIP6 - conducted with a range of ice sheet models, the projected 21st century sea level contribution differs significantly depending on these two factors. For the highest emission scenario RCP8.5, this leads to projected ice loss ranging from 1:4 to 4:0 cm of sea level equivalent in simulations in which ISMIP6 ocean forcing drives the PICO ocean box model where parameter tuning leads to a comparably low sub-shelf melt sensitivity and in which no surface forcing is applied. This is opposed to a likely range of 9:1 to 35:8 cm using the exact same initial setup, but emulated from the LARMIP-2 experiments with a higher melt sensitivity, even though both projects use forcing from climate models and melt rates are calibrated with previous oceanographic studies. Furthermore, using two initial states, one with a previous historic simulation from 1850 to 2014 and one starting from a steady state, we show that while differences between the ice sheet configurations in 2015 seem marginal at first sight, the historic simulation increases the susceptibility of the ice sheet to ocean warming, thereby increasing mass loss from 2015 to 2100 by 5% to 50 %. Hindcasting past ice sheet changes with numerical models would thus provide valuable tools to better constrain projections. Our results emphasize that the uncertainty that arises from the forcing is of the same order of magnitude as the ice dynamic response for future sea level projections.
Load partitioning between phases in a cast AlSi12CuMgNi alloy was investigated by in-situ compression test during neutron diffraction experiments. Computed tomography (CT) was used to determine volume fractions of eutectic Si and intermetallic (IM) phases, and to assess internal damage after ex-situ compression tests. The CT reconstructed volumes showed the interconnectivity of IM phases, which build a 3D network together with eutectic Si. Large stresses were found in IMs, revealing their significant role as a reinforcement for the alloy. An existing micromechanical model based on Maxwell scheme was extended to the present case, assuming the alloy as a three-phase composite (Al matrix, eutectic Si, IM phases). The model agrees well with the experimental data. Moreover, it allows predicting the principal stresses in each phase, while experiments can only determine stress differences between the axial and radial sample directions. Finally, we showed that the addition of alloying elements not only allowed developing a 3D interconnected network, but also improved the strength of the Al matrix, and the ability of the alloy constituents to bear mechanical load.
Arctic warming was more pronounced than warming in midlatitudes in the last decades making this region a hotspot of climate change. Associated with this, a rapid decline of sea-ice extent and a decrease of its thickness has been observed. Sea-ice retreat allows for an increased transport of heat and momentum from the ocean up to the tropo- and stratosphere by enhanced upward propagation of planetary-scale atmospheric waves. In the upper atmosphere, these waves deposit the momentum transported, disturbing the stratospheric polar vortex, which can lead to a breakdown of this circulation with the potential to also significantly impact the troposphere in mid- to late-winter and early spring. Therefore, an accurate representation of stratospheric processes in climate models is necessary to improve the understanding of the impact of retreating sea ice on the atmospheric circulation. By modeling the atmospheric response to a prescribed decline in Arctic sea ice, we show that including interactive stratospheric ozone chemistry in atmospheric model calculations leads to an improvement in tropo-stratospheric interactions compared to simulations without interactive chemistry. This suggests that stratospheric ozone chemistry is important for the understanding of sea ice related impacts on atmospheric dynamics.
The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field
(2017)
The interaction of gas phase endohedral fullerene Ho3N@C-80 with intense (0.1-5 x 10(14) W/cm(2)), short (30 fs), 800 nm laser pulses was investigated. The power law dependence of Ho3N@C-80(q+), q = 1-2, was found to be different from that of C-60. Time-dependent density functional theory computations revealed different light-induced ionization mechanisms. Unlike in C-60, in doped fullerenes, the breaking of the cage spherical symmetry makes super atomic molecular orbital (SAMO) states optically active. Theoretical calculations suggest that the fast ionization of the SAMO states in Ho3N@C-80 is responsible for the n = 3 power law for singly charged parent molecules at intensities lower than 1.2 x 10(14) W/cm(2).
Context. SMC AB6 is the shortest-period (P = 6.5 d) Wolf-Rayet (WR) binary in the Small Magellanic Cloud. This binary is therefore a key system in the study of binary interaction and formation of WR stars at low metallicity. The WR component in AB6 was previously found to be very luminous (log L = 6.3 [L-circle dot]) compared to its reported orbital mass (approximate to 8 M-circle dot), placing it significantly above the Eddington limit. Aims. Through spectroscopy and orbital analysis of newly acquired optical data taken with the Ultraviolet and Visual Echelle Spectrograph (UVES), we aim to understand the peculiar results reported for this system and explore its evolutionary history. Methods. We measured radial velocities via cross-correlation and performed a spectral analysis using the Potsdam Wolf-Rayet model atmosphere code. The evolution of the system was analyzed using the Binary Population and Spectral Synthesis evolution code. Results. AB6 contains at least four stars. The 6.5 d period WR binary comprises the WR primary (WN3:h, star A) and a rather rapidly rotating (v(eq) = 265 km s(-1)) early O-type companion (O5.5 V, star B). Static N III and N IV emission lines and absorption signatures in He lines suggest the presence of an early-type emission line star (O5.5 I(f), star C). Finally, narrow absorption lines portraying a long-term radial velocity variation show the existence of a fourth star (O7.5 V, star D). Star D appears to form a second 140 d period binary together with a fifth stellar member, which is a B-type dwarf or a black hole. It is not clear that these additional components are bound to the WR binary. We derive a mass ratio of M-O/M-WR = 2.2 +/- 0.1. The WR star is found to be less luminous than previously thought (log L = 5.9 [L-circle dot]) and, adopting M-O = 41 M-circle dot for star B, more massive (M-WR = 18 M-circle dot). Correspondingly, the WR star does not exceed the Eddington limit. We derive the initial masses of M-i,M-WR = 60 M-circle dot and M-i,M-O = 40 M-circle dot and an age of 3.9 Myr for the system. The WR binary likely experienced nonconservative mass transfer in the past supported by the relatively rapid rotation of star B. Conclusions. Our study shows that AB6 is a multiple - probably quintuple - system. This finding resolves the previously reported puzzle of the WR primary exceeding the Eddington limit and suggests that the WR star exchanged mass with its companion in the past.
We provide an abstract definition and an explicit construction of the stack of non-Abelian Yang-Mills fields on globally hyperbolic Lorentzian manifolds. We also formulate a stacky version of the Yang-Mills Cauchy problem and show that its well-posedness is equivalent to a whole family of parametrized PDE problems. Our work is based on the homotopy theoretical approach to stacks proposed in Hollander (Isr. J. Math. 163:93-124, 2008), which we shall extend by further constructions that are relevant for our purposes. In particular, we will clarify the concretification of mapping stacks to classifying stacks such as BG (con).
Context. NGC 253 is one of only two starburst galaxies found to emit gamma-rays from hundreds of MeV to multi-TeV energies. Accurate measurements of the very-high-energy (VHE; E> 100 GeV) and high-energy (HE; E > 60 MeV) spectra are crucial to study the underlying particle accelerators, probe the dominant emission mechanism(s) and to study cosmic-ray interaction and transport. Aims. The measurement of the VHE gamma-ray emission of NGC 253 published in 2012 by H.E.S.S. was limited by large systematic uncertainties. Here, the most up to date measurement of the gamma-ray spectrum of NGC 253 is investigated in both HE and VHE gamma-rays. Assuming a hadronic origin of the gamma-ray emission, the measurement uncertainties are propagated into the interpretation of the accelerated particle population. Methods. The data of H.E.S.S. observations are reanalysed using an updated calibration and analysis chain. The improved Fermi-LAT analysis employs more than 8 yr of data processed using pass 8. The cosmic-ray particle population is evaluated from the combined HE-VHE gamma-ray spectrum using NAIMA in the optically thin case. Results. The VHE gamma-ray energy spectrum is best fit by a power-law distribution with a flux normalisation of (1.34 +/- 0.14(stat) +/- 0.27(sys)) x 10(-13) cm(-2) s(-1) TeV-1 at 1 TeV - about 40% above, but compatible with the value obtained in Abramowski et al. (2012). The spectral index Gamma = 2.39 +/- 0.14(stat) +/- 0.25(sys) is slightly softer than but consistent with the previous measurement within systematic errors. In the Fermi energy range an integral flux of F(E > 60 MeV) = (1.56 +/- 0.28(stat) +/- 0.15(sys)) x 10(-8) cm(-2) s(-1) is obtained. At energies above similar to 3 GeV the HE spectrum is consistent with a power-law ranging into the VHE part of the spectrum measured by H.E.S.S. with an overall spectral index Gamma = 2.22 +/- 0.06(stat). Conclusions. Two scenarios for the starburst nucleus are tested, in which the gas in the starburst nucleus acts as either a thin or a thick target for hadronic cosmic rays accelerated by the individual sources in the nucleus. In these two models, the level to which NGC 253 acts as a calorimeter is estimated to a range of f(cal) = 0.1 to 1 while accounting for the measurement uncertainties. The presented spectrum is likely to remain the most accurate measurements until the Cherenkov Telescope Array (CTA) has collected a substantial set of data towards NGC 253.
The supernova remnant (SNR) W49B originated from a core-collapse supernova that occurred between one and four thousand years ago, and subsequently evolved into a mixed-morphology remnant, which is interacting with molecular clouds (MC). Gamma-ray observations of SNR-MC associations are a powerful tool to constrain the origin of Galactic cosmic rays, as they can probe the acceleration of hadrons through their interaction with the surrounding medium and subsequent emission of non-thermal photons. We report the detection of a gamma-ray source coincident with W49B at very high energies (VHE; E > 100 GeV) with the H.E.S.S. Cherenkov telescopes together with a study of the source with five years of Fermi-LAT high-energy gamma-ray (0.06-300 GeV) data. The smoothly connected, combined source spectrum, measured from 60 MeV to multi-TeV energies, shows two significant spectral breaks at 304 +/- 20 MeV and 8.4(-2.5)(+2.5) GeV; the latter is constrained by the joint fit from the two instruments. The detected spectral features are similar to those observed in several other SNR-MC associations and are found to be indicative of gamma-ray emission produced through neutral-pion decay.
Context:
Massive binaries play a crucial role in the Universe. Knowing the distributions of their orbital parameters is important for a wide range of topics from stellar feedback to binary evolution channels and from the distribution of supernova types to gravitational wave progenitors, yet no direct measurements exist outside the Milky Way.
Aims:
The Tarantula Massive Binary Monitoring project was designed to help fill this gap by obtaining multi-epoch radial velocity (RV) monitoring of 102 massive binaries in the 30 Doradus region.
Methods:
In this paper we analyze 32 FLAMES/GIRAFFE observations of 93 O- and 7 B-type binaries. We performed a Fourier analysis and obtained orbital solutions for 82 systems: 51 single-lined (SB1) and 31 double-lined (SB2) spectroscopic binaries.
Results:
Overall, the binary fraction and orbital properties across the 30 Doradus region are found to be similar to existing Galactic samples. This indicates that within these domains environmental effects are of second order in shaping the properties of massive binary systems. A small difference is found in the distribution of orbital periods, which is slightly flatter (in log space) in 30 Doradus than in the Galaxy, although this may be compatible within error estimates and differences in the fitting methodology. Also, orbital periods in 30 Doradus can be as short as 1.1 d, somewhat shorter than seen in Galactic samples. Equal mass binaries (q> 0.95) in 30 Doradus are all found outside NGC 2070, the central association that surrounds R136a, the very young and massive cluster at 30 Doradus’s core. Most of the differences, albeit small, are compatible with expectations from binary evolution. One outstanding exception, however, is the fact that earlier spectral types (O2–O7) tend to have shorter orbital periods than later spectral types (O9.2–O9.7).
Conclusions:
Our results point to a relative universality of the incidence rate of massive binaries and their orbital properties in the metallicity range from solar (Z⊙) to about half solar. This provides the first direct constraints on massive binary properties in massive star-forming galaxies at the Universe’s peak of star formation at redshifts z ~ 1 to 2 which are estimated to have Z ~ 0.5 Z⊙.
We present the first SB2 orbital solution and disentanglement of the massive Wolf-Rayet binary R145 (P = 159 d) located in the Large Magellanic Cloud. The primary was claimed to have a stellar mass greater than 300 M-circle dot, making it a candidate for being the most massive star known to date. While the primary is a known late-type, H-rich Wolf-Rayet star (WN6h), the secondary has so far not been unambiguously detected. Using moderate-resolution spectra, we are able to derive accurate radial velocities for both components. By performing simultaneous orbital and polarimetric analyses, we derive the complete set of orbital parameters, including the inclination. The spectra are disentangled and spectroscopically analyzed, and an analysis of the wind-wind collision zone is conducted. The disentangled spectra and our models are consistent with a WN6h type for the primary and suggest that the secondary is an O3.5 If*/WN7 type star. We derive a high eccentricity of e = 0 : 78 and minimum masses of M-1 sin(3) i approximate to M-2 sin(3) i = 13 +/- 2 M-circle dot, with q = M-2/M-1 = 1.01 +/- 0.07. An analysis of emission excess stemming from a wind-wind collision yields an inclination similar to that obtained from polarimetry (i = 39 +/- 6 degrees). Our analysis thus implies M-1 = 53(-20)(+40) and M2 = 54(-20)(+40) M-circle dot, excluding M-1 > 300 M-circle dot. A detailed comparison with evolution tracks calculated for single and binary stars together with the high eccentricity suggests that the components of the system underwent quasi-homogeneous evolution and avoided mass-transfer. This scenario would suggest current masses of approximate to 80 M-circle dot and initial masses of M-i,M-1 approximate to 10(5) and M-i,M-2 approximate to 90 M-circle dot, consistent with the upper limits of our derived orbital masses, and would imply an age of approximate to 2.2 Myr.
The time-dependent Schrödinger equation in non-integer dimensions for constrained quantum motion
(2020)
We propose a theoretical model, based on a generalized Schroedinger equation, to study the behavior of a constrained quantum system in non-integer, lower than two-dimensional space. The non-integer dimensional space is formed as a product space X x Y, comprising x-coordinate with a Hausdorff measure of dimension alpha(1) = D -1 (1 < D < 2) and y-coordinate with the Lebesgue measure of dimension of length (alpha(2) = 1). Geometric constraints are set at y = 0. Two different approaches to find the Green's function are employed, both giving the same form in terms of the Fox H-function. For D = 2, the solution for two-dimensional quantum motion on a comb is recovered. (C) 2020 Elsevier B.V. All rights reserved.
In the semiclassical limit (h) over bar -> 0, we analyze a class of self-adjoint Schrodinger operators H-(h) over bar = (h) over bar L-2 + (h) over barW + V center dot id(E) acting on sections of a vector bundle E over an oriented Riemannian manifold M where L is a Laplace type operator, W is an endomorphism field and the potential energy V has non-degenerate minima at a finite number of points m(1),... m(r) is an element of M, called potential wells. Using quasimodes of WKB-type near m(j) for eigenfunctions associated with the low lying eigenvalues of H-(h) over bar, we analyze the tunneling effect, i.e. the splitting between low lying eigenvalues, which e.g. arises in certain symmetric configurations. Technically, we treat the coupling between different potential wells by an interaction matrix and we consider the case of a single minimal geodesic (with respect to the associated Agmon metric) connecting two potential wells and the case of a submanifold of minimal geodesics of dimension l + 1. This dimension l determines the polynomial prefactor for exponentially small eigenvalue splitting.
We study the hierarchical stellar structures in a similar to 1.5 deg(2) area covering the 30. Doradus-N158-N159-N160 starforming complex with the VISTA Survey of. Magellanic Clouds. Based on the young upper main-sequence stars, we find that the surface densities cover a wide range of values, from log(Sigma.pc(2))less than or similar to -2.0 to log(Sigma. pc(2)) greater than or similar to 0.0. Their distributions are highly non-uniform, showing groups that frequently have subgroups inside. The sizes of the stellar groups do not exhibit characteristic values, and range continuously from several parsecs to more than 100. pc; the cumulative size distribution can be well described by a single power law, with the power-law index indicating a projected fractal dimension D-2 = 1.6 +/- 0.3. We suggest that the phenomena revealed here support a scenario of hierarchical star formation. Comparisons with other star-forming regions and galaxies are also discussed.
Context. Massive Wolf-Rayet (WR) stars dominate the radiative and mechanical energy budget of galaxies and probe a critical phase in the evolution of massive stars prior to core collapse. It is not known whether core He-burning WR stars (classical WR; cWR) form predominantly through wind stripping (w-WR) or binary stripping (b-WR). Whereas spectroscopy of WR binaries has so-far largely been avoided because of its complexity, our study focuses on the 44 WR binaries and binary candidates of the Large Magellanic Cloud (LMC; metallicity Z approximate to 0.5 Z(circle dot)), which were identified on the basis of radial velocity variations, composite spectra, or high X-ray luminosities. Aims. Relying on a diverse spectroscopic database, we aim to derive the physical and orbital parameters of our targets, confronting evolution models of evolved massive stars at subsolar metallicity and constraining the impact of binary interaction in forming these stars. Methods. Spectroscopy was performed using the Potsdam Wolf-Rayet (PoWR) code and cross-correlation techniques. Disentanglement was performed using the code Spectangular or the shift-and-add algorithm. Evolutionary status was interpreted using the Binary Population and Spectral Synthesis (BPASS) code, exploring binary interaction and chemically homogeneous evolution. Results. Among our sample, 28/44 objects show composite spectra and are analyzed as such. An additional five targets show periodically moving WR primaries but no detected companions (SB1); two (BAT99 99 and 112) are potential WR + compact-object candidates owing to their high X-ray luminosities. We cannot confirm the binary nature of the remaining 11 candidates. About two-thirds of the WN components in binaries are identified as cWR, and one-third as hydrogen-burning WR stars. We establish metallicity-dependent mass-loss recipes, which broadly agree with those recently derived for single WN stars, and in which so-called WN3/O3 stars are clear outliers. We estimate that 45 +/- 30% of the cWR stars in our sample have interacted with a companion via mass transfer. However, only approximate to 12 +/- 7% of the cWR stars in our sample naively appear to have formed purely owing to stripping via a companion (12% b-WR). Assuming that apparently single WR stars truly formed as single stars, this comprises approximate to 4% of the whole LMC WN population, which is about ten times less than expected. No obvious differences in the properties of single and binary WN stars, whose luminosities extend down to log L approximate to 5.2 [L-circle dot], are apparent. With the exception of a few systems (BAT99 19, 49, and 103), the equatorial rotational velocities of the OB-type companions are moderate (v(eq) less than or similar to 250 km s(-1)) and challenge standard formalisms of angular-momentum accretion. For most objects, chemically homogeneous evolution can be rejected for the secondary, but not for the WR progenitor. Conclusions. No obvious dichotomy in the locations of apparently single and binary WN stars on the Hertzsprung-Russell diagram is apparent. According to commonly used stellar evolution models (BPASS, Geneva), most apparently single WN stars could not have formed as single stars, implying that they were stripped by an undetected companion. Otherwise, it must follow that pre-WR mass-loss/mixing (e.g., during the red supergiant phase) are strongly underestimated in standard stellar evolution models.
In this work we present spectra of all gamma-ray burst (GRB) afterglows that have been promptly observed with the X-shooter spectrograph until 31/03/2017. In total, we have obtained spectroscopic observations of 103 individual GRBs observed within 48 hours of the GRB trigger. Redshifts have been measured for 97 per cent of these, covering a redshift range from 0.059 to 7.84. Based on a set of observational selection criteria that minimise biases with regards to intrinsic properties of the GRBs, the follow-up effort has been focused on producing a homogeneously selected sample of 93 afterglow spectra for GRBs discovered by the Swift satellite. We here provide a public release of all the reduced spectra, including continuum estimates and telluric absorption corrections. For completeness, we also provide reductions for the 18 late-time observations of the underlying host galaxies. We provide an assessment of the degree of completeness with respect to the parent GRB population, in terms of the X-ray properties of the bursts in the sample and find that the sample presented here is representative of the full Swift sample. We have constrained the fraction of dark bursts to be <28 per cent and confirm previous results that higher optical darkness is correlated with increased X-ray absorption. For the 42 bursts for which it is possible, we have provided a measurement of the neutral hydrogen column density, increasing the total number of published HI column density measurements by similar to 33 per cent. This dataset provides a unique resource to study the ISM across cosmic time, from the local progenitor surroundings to the intervening Universe.
Fast, three-dimensional polarization mapping in piezoelectric sensor cables was performed by means of the novel thermal-pulse tomography (TPT) technique with a lateral resolution of 200 mum. The active piezoelectric cable material (a copolymer of polyvinylidene fluoride with trifluoroethylene) was electrically poled with a point-to-cable corona discharge. A focused laser was employed to heat the opaque outer electrode, and the short-circuit current generated by the thermal pulse was used to obtain 3D polarization maps via the scale transformation method. The article describes the TPT technique as a fast non-destructive option for studying cylindrical geometries.
We characterize finite-time thermodynamic processes of multidimensional quadratic overdamped systems.
Analytic expressions are provided for heat, work, and dissipation for any evolution of the system covariance matrix.
The Bures-Wasserstein metric between covariance matrices naturally emerges as the local quantifier of dissipation.
General principles of how to apply these geometric tools to identify optimal protocols are discussed.
Focusing on the relevant slow-driving limit, we show how these results can be used to analyze cases in which the experimental control over the system is partial.
How different microscopic mechanisms of ultrafast spin dynamics coexist and interplay is not only relevant for the development of spintronics but also for the thorough description of physical systems out-of-equilibrium. In pure crystalline ferromagnets, one of the main microscopic mechanism of spin relaxation is the electron-phonon (el-ph) driven spin-flip, or Elliott-Yafet, scattering. Unexpectedly, recent experiments with ferro- and ferrimagnetic alloys have shown different dynamics for the different sublattices. These distinct sublattice dynamics are contradictory to the Elliott-Yafet scenario. In order to rationalize this discrepancy, it has been proposed that the intra- and intersublattice exchange interaction energies must be considered in the microscopic demagnetization mechanism, too. Here, using a temperature-dependent x-ray emission spectroscopy (XES) method, we address experimentally the element specific el-ph angular momentum transfer rates, responsible for the spin-flips in the respective (sub)lattices of Fe20Ni80, Fe50Ni50 and pure nickel single crystals. We establish how the deduced rate evolution with the temperature is linked to the exchange coupling constants reported for different alloy stoichiometries and how sublattice exchange energies threshold the related el-ph spin-flip channels. Thus, these results evidence that the Elliott-Yafet spin-flip scattering, thresholded by sublattice exchange energies, is the relevant microscopic process to describe sublattice dynamics in alloys and elemental magnetic systems.
How ergodic is diffusion under harmonic confinements? How strongly do ensemble- and time-averaged displacements differ for a thermally-agitated particle performing confined motion for different initial conditions? We here study these questions for the generic Ornstein-Uhlenbeck (OU) process and derive the analytical expressions for the second and fourth moment. These quantifiers are particularly relevant for the increasing number of single-particle tracking experiments using optical traps. For a fixed starting position, we discuss the definitions underlying the ensemble averages. We also quantify effects of equilibrium and nonequilibrium initial particle distributions onto the relaxation properties and emerging nonequivalence of the ensemble- and time-averaged displacements (even in the limit of long trajectories). We derive analytical expressions for the ergodicity breaking parameter quantifying the amplitude scatter of individual time-averaged trajectories, both for equilibrium and outof-equilibrium initial particle positions, in the entire range of lag times. Our analytical predictions are in excellent agreement with results of computer simulations of the Langevin equation in a parabolic potential. We also examine the validity of the Einstein relation for the ensemble- and time-averaged moments of the OU-particle. Some physical systems, in which the relaxation and nonergodic features we unveiled may be observable, are discussed.
How different are the results of constant-rate resetting of anomalous-diffusion processes in terms of their ensemble-averaged versus time-averaged mean-squared displacements (MSDs versus TAMSDs) and how does stochastic resetting impact nonergodicity? We examine, both analytically and by simulations, the implications of resetting on the MSD- and TAMSD-based spreading dynamics of particles executing fractional Brownian motion (FBM) with a long-time memory, heterogeneous diffusion processes (HDPs) with a power-law space-dependent diffusivity D(x) = D0|x|gamma and their "combined" process of HDP-FBM. We find, inter alia, that the resetting dynamics of originally ergodic FBM for superdiffusive Hurst exponents develops disparities in scaling and magnitudes of the MSDs and mean TAMSDs indicating weak ergodicity breaking. For subdiffusive HDPs we also quantify the nonequivalence of the MSD and TAMSD and observe a new trimodal form of the probability density function. For reset FBM, HDPs and HDP-FBM we compute analytically and verify by simulations the short-time MSD and TAMSD asymptotes and long-time plateaus reminiscent of those for processes under confinement. We show that certain characteristics of these reset processes are functionally similar despite a different stochastic nature of their nonreset variants. Importantly, we discover nonmonotonicity of the ergodicitybreaking parameter EB as a function of the resetting rate r. For all reset processes studied we unveil a pronounced resetting-induced nonergodicity with a maximum of EB at intermediate r and EB similar to(1/r )-decay at large r. Alongside the emerging MSD-versus-TAMSD disparity, this r-dependence of EB can be an experimentally testable prediction. We conclude by discussing some implications to experimental systems featuring resetting dynamics.
We introduce three strategies for the analysis of financial time series based on time averaged observables. These comprise the time averaged mean squared displacement (MSD) as well as the ageing and delay time methods for varying fractions of the financial time series. We explore these concepts via statistical analysis of historic time series for several Dow Jones Industrial indices for the period from the 1960s to 2015. Remarkably, we discover a simple universal law for the delay time averaged MSD. The observed features of the financial time series dynamics agree well with our analytical results for the time averaged measurables for geometric Brownian motion, underlying the famed Black–Scholes–Merton model. The concepts we promote here are shown to be useful for financial data analysis and enable one to unveil new universal features of stock market dynamics.
We investigate the effects of a time-delayed all-to-all coupling scheme in a large population of oscillators with natural frequencies following a bimodal distribution. The regions of parameter space corresponding to synchronized and incoherent solutions are obtained both numerically and analytically for particular frequency distributions. In particular, we find that bimodality introduces a new time scale that results in a quasiperiodic disposition of the regions of incoherence.
How do near-bankruptcy events in the past affect the dynamics of stock-market prices in the future? Specifically, what are the long-time properties of a time-local exponential growth of stock-market prices under the influence of stochastically occurring economic crashes? Here, we derive the ensemble- and time-averaged properties of the respective "economic" or geometric Brownian motion (GBM) with a nonzero drift exposed to a Poissonian constant-rate price-restarting process of "resetting." We examine-based both on thorough analytical calculations and on findings from systematic stochastic computer simulations-the general situation of reset GBM with a nonzero [positive] drift and for all special cases emerging for varying parameters of drift, volatility, and reset rate in the model. We derive and summarize all short- and long-time dependencies for the mean-squared displacement (MSD), the variance, and the mean time-averaged MSD (TAMSD) of the process of Poisson-reset GBM under the conditions of both rare and frequent resetting. We consider three main regions of model parameters and categorize the crossovers between different functional behaviors of the statistical quantifiers of this process. The analytical relations are fully supported by the results of computer simulations. In particular, we obtain that Poisson-reset GBM is a nonergodic stochastic process, with generally MSD(Delta) not equal TAMSD(Delta) and Variance(Delta) not equal TAMSD(Delta) at short lag times Delta and for long trajectory lengths T. We investigate the behavior of the ergodicity-breaking parameter in each of the three regions of parameters and examine its dependence on the rate of reset at Delta/T << 1. Applications of these theoretical results to the analysis of prices of reset-containing options are pertinent.
Time-resolved crystallography reveals allosteric communication aligned with molecular breathing
(2019)
A comprehensive understanding of protein function demands correlating structure and dynamic changes. Using time-resolved serial synchrotron crystallography, we visualized half-of-the-sites reactivity and correlated molecular-breathing motions in the enzyme fluoroacetate dehalogenase. Eighteen time points from 30 milliseconds to 30 seconds cover four turnover cycles of the irreversible reaction. They reveal sequential substrate binding, covalent-intermediate formation, setup of a hydrolytic water molecule, and product release. Small structural changes of the protein mold and variations in the number and placement of water molecules accompany the various chemical steps of catalysis. Triggered by enzyme-ligand interactions, these repetitive changes in the protein framework’s dynamics and entropy constitute crucial components of the catalytic machinery.
The prototypical photoinduced dissociation of Fe(CO)(5) in the gas phase is used to test time-resolved x-ray photoelectron spectroscopy for studying photochemical reactions. Upon one-photon excitation at 266 nm, Fe(CO)(5) successively dissociates to Fe(CO)(4) and Fe(CO)(3) along a pathway where both fragments retain the singlet multiplicity of Fe(CO)(5). The x-ray free-electron laser FLASH is used to probe the reaction intermediates Fe(CO)(4) and Fe(CO)(3) with time-resolved valence and core-level photoelectron spectroscopy, and experimental results are interpreted with ab initio quantum chemical calculations. Changes in the valence photoelectron spectra are shown to reflect changes in the valenceorbital interactions upon Fe-CO dissociation, thereby validating fundamental theoretical concepts in Fe-CO bonding. Chemical shifts of CO 3 sigma inner-valence and Fe 3 sigma core-level binding energies are shown to correlate with changes in the coordination number of the Fe center. We interpret this with coordination-dependent charge localization and core-hole screening based on calculated changes in electron densities upon core-hole creation in the final ionic states. This extends the established capabilities of steady-state electron spectroscopy for chemical analysis to time-resolved investigations. It could also serve as a benchmark for howcharge and spin density changes in molecular dissociation and excited-state dynamics are expressed in valence and core-level photoelectron spectroscopy. Published by AIP Publishing.
A new variant of the Laser-Induced Pressure-Pulse (LIPP) method for repeatable, time-resolved space-charge profile measurements is proposed and demonstrated. Automated deposition of a fresh laser-target film before each illumination leads to good repeatability of the LIPP and thus allows for the detection of time-resolved changes in the space-charge distribution over many hours. We describe and discuss the experimental setup and its features, compare the repeatability of the LIPP measurements on the same sample without and with re-preparation of the test cell, and present the time-resolved evolution of the space-charge profile in a two-layer arrangement of a silicone-grease and a silicone-elastomer film as an example. Finally, the temperature dependence of the space-charge evolution during polarization under high voltage and during depolarization in short circuit is shown. Possible uses and future developments of the new LIPP approach are also discussed.
Modern stationary X-ray spectroscopy is unable to resolve rotational structure.
In the present paper, we propose to use time-resolved two color X-ray pump-probe spectroscopy with picosecond resolution for real-time monitoring of the rotational dynamics induced by the recoil effect.
The proposed technique consists of two steps.
The first short pump X-ray pulse ionizes the valence electron, which transfers angular momentum to the molecule.
The second time-delayed short probe X-ray pulse resonantly excites a 1s electron to the created valence hole.
Due to the recoil-induced angular momentum the molecule rotates and changes the orientation of transition dipole moment of core-excitation with respect to the transition dipole moment of the valence ionization, which results in a temporal modulation of the probe X-ray absorption as a function of the delay time between the pulses.
We developed an accurate theory of the X-ray pump-probe spectroscopy of the recoil-induced rotation and study how the energy of the photoelectron and thermal dephasing affect the structure of the time-dependent X-ray absorption using the CO molecule as a case-study.
We also discuss the feasibility of experimental observation of our theoretical findings, opening new perspectives in studies of molecular rotational dynamics.
The electric field-dependence of structural dynamics in a tetragonal ferroelectric lead zirconate titanate thin film is investigated under subcoercive and above-coercive fields using time-resolved X-ray diffraction. The domain nucleation and growth are monitored in real time during the application of an external field to the prepoled thin film capacitor. We propose the observed broadening of the in-plane peak width of the symmetric 002 Bragg reflection as an indicator of the domain disorder and discuss the processes that change the measured peak intensity. Subcoercive field switching results in remnant disordered domain configurations. Published under license by AIP Publishing.
We show that the equation proposed by Takeuchi and Argon to explain the creep behavior of Al-Mg solid solution can be used to describe also the creep behavior of pure aluminum. In this frame, it is possible to avoid the use of the classic pre-exponential fitting parameter in the power law equation to predict the minimum creep strain rate. The effect of the fractal arrangement of dislocations, developed at the mesoscale, must be considered to fully explain the experimental data. These ideas allow improving the recently introduced SSTC model, fully describing the primary and secondary creep regimes of aluminum alloys without the need for fitting. Creep data from commercially pure A199.8% and Al-Mg alloys tested at different temperatures and stresses are used to validate the proposed ideas.
Towards a full quantitative description of single-molecule reaction kinetics in biological cells
(2018)
The first-passage time (FPT), i.e., the moment when a stochastic process reaches a given threshold value for the first time, is a fundamental mathematical concept with immediate applications. In particular, it quantifies the statistics of instances when biomolecules in a biological cell reach their specific binding sites and trigger cellular regulation. Typically, the first-passage properties are given in terms of mean first-passage times. However, modern experiments now monitor single-molecular binding-processes in living cells and thus provide access to the full statistics of the underlying first-passage events, in particular, inherent cell-to-cell fluctuations. We here present a robust explicit approach for obtaining the distribution of FPTs to a small partially reactive target in cylindrical-annulus domains, which represent typical bacterial and neuronal cell shapes. We investigate various asymptotic behaviours of this FPT distribution and show that it is typically very broad in many biological situations, thus, the mean FPT can differ from the most probable FPT by orders of magnitude. The most probable FPT is shown to strongly depend only on the starting position within the geometry and to be almost independent of the target size and reactivity. These findings demonstrate the dramatic relevance of knowing the full distribution of FPTs and thus open new perspectives for a more reliable description of many intracellular processes initiated by the arrival of one or few biomolecules to a small, spatially localised region inside the cell.
Anomalous-diffusion, the departure of the spreading dynamics of diffusing particles from the traditional law of Brownian-motion, is a signature feature of a large number of complex soft-matter and biological systems. Anomalous-diffusion emerges due to a variety of physical mechanisms, e.g., trapping interactions or the viscoelasticity of the environment. However, sometimes systems dynamics are erroneously claimed to be anomalous, despite the fact that the true motion is Brownian—or vice versa. This ambiguity in establishing whether the dynamics as normal or anomalous can have far-reaching consequences, e.g., in predictions for reaction- or relaxation-laws. Demonstrating that a system exhibits normal- or anomalous-diffusion is highly desirable for a vast host of applications. Here, we present a criterion for anomalous-diffusion based on the method of power-spectral analysis of single trajectories. The robustness of this criterion is studied for trajectories of fractional-Brownian-motion, a ubiquitous stochastic process for the description of anomalous-diffusion, in the presence of two types of measurement errors. In particular, we find that our criterion is very robust for subdiffusion. Various tests on surrogate data in absence or presence of additional positional noise demonstrate the efficacy of this method in practical contexts. Finally, we provide a proof-of-concept based on diverse experiments exhibiting both normal and anomalous-diffusion.
Using time-resolved x-ray diffraction, we demonstrate the manipulation of the picosecond strain response of a metallic heterostructure consisting of a dysprosium (Dy) transducer and a niobium (Nb) detection layer by an external magnetic field. We utilize the first-order ferromagnetic–antiferromagnetic phase transition of the Dy layer, which provides an additional large contractive stress upon laser excitation compared to its zerofield response. This enhances the laser-induced contraction of the transducer and changes the shape of the picosecond strain pulses driven in Dy and detected within the buried Nb layer. Based on our experiment with rare-earth metals we discuss required properties for functional transducers, which may allow for novel field-control of the emitted picosecond strain pulses.
We combine ultrafast X-ray diffraction (UXRD) and time-resolved Magneto-Optical Kerr Effect (MOKE) measurements to monitor the strain pulses in laser-excited TbFe2/Nb heterostructures. Spatial separation of the Nb detection layer from the laser excitation region allows for a background-free characterization of the laser-generated strain pulses. We clearly observe symmetric bipolar strain pulses if the excited TbFe2 surface terminates the sample and a decomposition of the strain wavepacket into an asymmetric bipolar and a unipolar pulse, if a SiO2 glass capping layer covers the excited TbFe2 layer. The inverse magnetostriction of the temporally separated unipolar strain pulses in this sample leads to a MOKE signal that linearly depends on the strain pulse amplitude measured through UXRD. Linear chain model simulations accurately predict the timing and shape of UXRD and MOKE signals that are caused by the strain reflections from multiple interfaces in the heterostructure.
The European potential for renewable electricity is sufficient to enable fully renewable supply on different scales, from self-sufficient, subnational regions to an interconnected continent. We not only show that a continental-scale system is the cheapest, but also that systems on the national scale and below are possible at cost penalties of 20% or less. Transmission is key to low cost, but it is not necessary to vastly expand the transmission system. When electricity is transmitted only to balance fluctuations, the transmission grid size is comparable to today's, albeit with expanded cross-border capacities. The largest differences across scales concern land use and thus social acceptance: in the continental system, generation capacity is concentrated on the European periphery, where the best resources are. Regional systems, in contrast, have more dispersed generation. The key trade-off is therefore not between geographic scale and cost, but between scale and the spatial distribution of required generation and transmission infrastructure.
We explore the risk that self-reinforcing feedbacks could push the Earth System toward a planetary threshold that, if crossed, could prevent stabilization of the climate at intermediate temperature rises and cause continued warming on a "Hothouse Earth" pathway even as human emissions are reduced. Crossing the threshold would lead to a much higher global average temperature than any interglacial in the past 1.2 million years and to sea levels significantly higher than at any time in the Holocene. We examine the evidence that such a threshold might exist and where it might be. If the threshold is crossed, the resulting trajectory would likely cause serious disruptions to ecosystems, society, and economies. Collective human action is required to steer the Earth System away from a potential threshold and stabilize it in a habitable interglacial-like state. Such action entails stewardship of the entire Earth System-biosphere, climate, and societies-and could include decarbonization of the global economy, enhancement of biosphere carbon sinks, behavioral changes, technological innovations, new governance arrangements, and transformed social values.
We perform a detailed statistical analysis of diffusive trajectories of membrane-enclosed vesicles (vacuoles) in the supercrowded cytoplasm of living Acanthamoeba castellanii cells. From the vacuole traces recorded in the center-of-area frame of moving amoebae, we examine the statistics of the time-averaged mean-squared displacements of vacuoles, their generalized diffusion coefficients and anomalous scaling exponents, the ergodicity breaking parameter, the non-Gaussian features of displacement distributions of vacuoles, the displacement autocorrelation function, as well as the distributions of speeds and positions of vacuoles inside the amoeba cells. Our findings deliver novel insights into the internal dynamics of cellular structures in these infectious pathogens. Published under license by AIP Publishing.
Transition path dynamics have been widely studied in chemical, physical, and technological systems. Mostly, the transition path dynamics is obtained for smooth barrier potentials, for instance, generic inverse-parabolic shapes. We here present analytical results for the mean transition path time, the distribution of transition path times, the mean transition path velocity, and the mean transition path shape in a rough inverted parabolic potential function under the driving of Gaussian white noise. These are validated against extensive simulations using the forward flux sampling scheme in parallel computations. We observe how precisely the potential roughness, the barrier height, and the noise intensity contribute to the particle transition in the rough inverted barrier potential.
We present an alternative approach to finite-size effects around the synchronization transition in the standard Kuramoto model. Our main focus lies on the conditions under which a collective oscillatory mode is well defined. For this purpose, the minimal value of the amplitude of the complex Kuramoto order parameter appears as a proper indicator. The dependence of this minimum on coupling strength varies due to sampling variations and correlates with the sample kurtosis of the natural frequency distribution. The skewness of the frequency sample determines the frequency of the resulting collective mode. The effects of kurtosis and skewness hold in the thermodynamic limit of infinite ensembles. We prove this by integrating a self-consistency equation for the complex Kuramoto order parameter for two families of distributions with controlled kurtosis and skewness, respectively.
We investigate the transition from incoherence to global collective motion in a three-dimensional swarming model of agents with helical trajectories, subject to noise and global coupling. Without noise this model was recently proposed as a generalization of the Kuramoto model and it was found that alignment of the velocities occurs discontinuously for arbitrarily small attractive coupling. Adding noise to the system resolves this singular limit and leads to a continuous transition, either to a directed collective motion or to center-of-mass rotations.
I study deterministic dynamics of chiral active particles in two dimensions. Particles are considered as discs interacting with elastic repulsive forces. An ensemble of particles, started from random initial conditions, demonstrates chaotic collisions resulting in their normal diffusion. This chaos is transient, as rather abruptly a synchronous collisionless state establishes. The life time of chaos grows exponentially with the number of particles. External forcing (periodic or chaotic) is shown to facilitate the synchronization transition.
Transport in exclusion processes with one-step memory: density dependence and optimal acceleration
(2019)
We study a lattice gas of persistent walkers, in which each site is occupied by at most one particle and the direction each particle attempts to move to depends on its last step. We analyse the mean squared displacement (MSD) of the particles as a function of the particle density and their persistence (the tendency to continue moving in the same direction). For positive persistence the MSD behaves as expected: it increases with the persistence and decreases with the density. However, for strong anti-persistence we find two different regimes, in which the dependence of the MSD on the density is non-monotonic. For very strong anti-persistence there is an optimal density at which the MSD reaches a maximum. In an intermediate regime, the MSD as a function of the density exhibits both a minimum and a maximum, a phenomenon which has not been observed before. We derive a mean-field theory which qualitatively explains this behaviour.
Using magneto-optical Faraday and Kerr measurements, we investigate the magnetic and magnetooptical properties of a thick Bi-substituted gadolinium iron garnet film over a broad range of wavelengths (250-850 nm) and temperatures (150-300 K), including the magnetization compensation point, TM. We observe an exchange-bias-like effect in the vicinity of TM. By slightly changing the sample temperature, we can precisely tune the bias field, which reaches a magnitude 6 times higher than the coercive field. We explain this phenomenon by considering the short-range superexchange interaction and a change in the magnetic behavior when moving from the surface to the bulk of the film. This finding may lead to the development of single-film magneto-optical devices based on the exchange-bias effect.
The application of the fractional calculus in the mathematical modelling of relaxation processes in complex heterogeneous media has attracted a considerable amount of interest lately.
The reason for this is the successful implementation of fractional stochastic and kinetic equations in the studies of non-Debye relaxation.
In this work, we consider the rotational diffusion equation with a generalised memory kernel in the context of dielectric relaxation processes in a medium composed of polar molecules. We give an overview of existing models on non-exponential relaxation and introduce an exponential resetting dynamic in the corresponding process.
The autocorrelation function and complex susceptibility are analysed in detail.
We show that stochastic resetting leads to a saturation of the autocorrelation function to a constant value, in contrast to the case without resetting, for which it decays to zero. The behaviour of the autocorrelation function, as well as the complex susceptibility in the presence of resetting, confirms that the dielectric relaxation dynamics can be tuned by an appropriate choice of the resetting rate.
The presented results are general and flexible, and they will be of interest for the theoretical description of non-trivial relaxation dynamics in heterogeneous systems composed of polar molecules.
The recent development of donor–acceptor copolymers has led to an enormous improvement in the performance of organic solar cells and organic field-effect transistors. Here we describe the synthesis, detailed characterisation, and application of a series of structurally modified copolymers to investigate fundamental structure–property relationships in this class of conjugated polymers. The interplay between chemical structure and optoelectronic properties is investigated. These are further correlated to the charge transport and solar cell performance, which allows us to link their chemical structure to the observed physical properties.