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Synthesis of organic-inorganic hybrids based on the conjugated polymer P3HT and mesoporous silicon
(2022)
Organic-inorganic hybrids are a class of functional materials that combine favorable properties of their constituents to achieve an overall improved performance for a wide range of applications. This article presents the synthesis route for P3HT-porous silicon hybrids for thermoelectric applications. The conjugated polymer P3HT is incorporated into the porous silicon matrix by means of melt infiltration. Gravimetry, sorption isotherms and energy dispersive X-ray spectroscopy (EDX) mapping indicate that the organic molecules occupy more than 50% of the void space in the inorganic host. We demonstrate that subsequent diffusion-based doping of the confined polymer in a FeCl3 solution increases the electrical conductivity of the hybrid by five orders of magnitude compared to the empty porous silicon host.
This article presents inelastic thermal neutron scattering experiments probing the phonon dispersion in mesoporous silicon with pores 8 nm across. Scattering studies reveal the energy-momentum relation for transverse and longitudinal phonons along the high symmetry directions , and in the Brillouin zone. The dispersion up to phonon energies of 35 meV unambiguously proves that the phonon group velocities in highly-crystalline silicon are not modified by nanostructuring down to sub-10 nanometer length scales. On these length scales, there is apparently no effect of structuring on the elastic moduli of mesoporous silicon. No evidence can be found for phonon-softening in topologically complex, geometrically disordered mesoporous silicon putting it in contrast to silicon nanotubes and nanoribbons.
We consider sedimented at a solid wall particles that are immersed in water containing small additives of photosensitive ionic surfactants. It is shown that illumination with an appropriate wavelength, a beam intensity profile, shape and size could lead to a variety of dynamic, both unsteady and steady state, configurations of particles. These dynamic, well-controlled and switchable particle patterns at the wall are due to an emerging diffusio-osmotic flow that takes its origin in the adjacent to the wall electrostatic diffuse layer, where the concentration gradients of surfactant are induced by light. The conventional nonporous particles are passive and can move only with already generated flow. However, porous colloids actively participate themselves in the flow generation mechanism at the wall, which also sets their interactions that can be very long ranged. This light-induced diffusio-osmosis opens novel avenues to manipulate colloidal particles and assemble them to various patterns. We show in particular how to create and split optically the confined regions of particles of tunable size and shape, where well-controlled flow-induced forces on the colloids could result in their crystalline packing, formation of dilute lattices of well-separated particles, and other states.
Materials realizing the XY model in two dimensions are sparse.
Here we use neutron triple-axis spectroscopy to investigate the critical static and dynamical magnetic fluctuations in the square-lattice antiferromagnets Ca2RuO4 and Ca3Ru2O7.
We probe the temperature dependence of the antiferromagnetic Bragg intensity, the Q width, the amplitude, and the energy width of the magnetic diffuse scattering in the vicinity of the Neel temperature T-N to determine the critical behavior of the magnetic order parameter M, correlation length xi, susceptibility chi, and the characteristic energy Gamma with the corresponding critical exponents beta, nu, gamma, and z, respectively.
We find that the critical behaviors of the single-layer compound Ca2RuO4 follow universal scaling laws that are compatible with predictions of the two-dimensional (2D) XY model.
The bilayer compound Ca3Ru2O7 is only partly consistent with the 2D XY theory and best described by the three-dimensional (3D) Ising model, which is likely a consequence of the intrabilayer exchange interactions in combination with an orthorhombic single-ion anisotropy.
Hence, our results suggest that layered ruthenates are promising solid-state platforms for research on the 2D XY model and the effects of 3D interactions and additional spin-space anisotropies on the magnetic fluctuations.
In star-forming galaxies, the far-infrared (FIR) and radio-continuum luminosities obey a tight empirical relation over a large range of star-formation rates (SFR).
To understand the physics, we examine magnetohydrodynamic galaxy simulations, which follow the genesis of cosmic ray (CR) protons at supernovae and their advective and anisotropic diffusive transport.
We show that gravitational collapse of the proto-galaxy generates a corrugated accretion shock, which injects turbulence and drives a small-scale magnetic dynamo. As the shock propagates outwards and the associated turbulence decays, the large velocity shear between the supersonically rotating cool disc with respect to the (partially) pressure-supported hot circumgalactic medium excites Kelvin-Helmholtz surface and body modes.
Those interact non-linearly, inject additional turbulence and continuously drive multiple small-scale dynamos, which exponentially amplify weak seed magnetic fields.
After saturation at small scales, they grow in scale to reach equipartition with thermal and CR energies in Milky Way-mass galaxies. In small galaxies, the magnetic energy saturates at the turbulent energy while it fails to reach equipartition with thermal and CR energies.
We solve for steady-state spectra of CR protons, secondary electrons/positrons from hadronic CR-proton interactions with the interstellar medium, and primary shock-accelerated electrons at supernovae.
The radio-synchrotron emission is dominated by primary electrons, irradiates the magnetized disc and bulge of our simulated Milky Way-mass galaxy and weakly traces bubble-shaped magnetically loaded outflows.
Our star-forming and star-bursting galaxies with saturated magnetic fields match the global FIR-radio correlation (FRC) across four orders of magnitude. Its intrinsic scatter arises due to (i) different magnetic saturation levels that result from different seed magnetic fields, (ii) different radio synchrotron luminosities for different specific SFRs at fixed SFR, and (iii) a varying radio intensity with galactic inclination.
In agreement with observations, several 100-pc-sized regions within star-forming galaxies also obey the FRC, while the centres of starbursts substantially exceed the FRC.
In this topical review, we give an overview of the structure and dynamics of a single polymer chain in active baths, Gaussian or non-Gaussian.
The review begins with the discussion of single flexible or semiflexible linear polymer chains subjected to two noises, thermal and active.
The active noise has either Gaussian or non-Gaussian distribution but has a memory, accounting for the persistent motion of the active bath particles. This finite persistence makes the reconfiguration dynamics of the chain slow as compared to the purely thermal case and the chain swells.
The active noise also results superdiffusive or ballistic motion of the tagged monomer. We present all the calculations in details but mainly focus on the analytically exact or almost exact results on the topic, as obtained from our group in recent years.
In addition, we briefly mention important works of other groups and include some of our new results. The review concludes with pointing out the implications of polymer chains in active bath in biologically relevant context and its future directions.
How predictable is the next move of an animal? Specifically, which factors govern the short- and long-term motion patterns and the overall dynamics of land-bound, plant-eating animals in general and ruminants in particular? To answer this question, we here study the movement dynamics of springbok antelopes Antidorcas marsupialis. We propose several complementary statistical-analysis techniques combined with machine-learning approaches to analyze—across multiple time scales—the springbok motion recorded in long-term GPS tracking of collared springboks at a private wildlife reserve in Namibia. As a result, we are able to predict the springbok movement within the next hour with a certainty of about 20%. The remaining about 80% are stochastic in nature and are induced by unaccounted factors in the modeling algorithm and by individual behavioral features of springboks. We find that directedness of motion contributes approximately 17% to this predicted fraction. We find that the measure for directedeness is strongly dependent on the daily cycle of springbok activity. The previously known daily affinity of springboks to their water points, as predicted from our machine-learning algorithm, overall accounts for only about 3% of this predicted deterministic component of springbok motion. Moreover, the resting points are found to affect the motion of springboks at least as much as the formally studied effects of water points. The generality of these statements for the motion patterns and their underlying behavioral reasons for other ruminants can be examined on the basis of our statistical-analysis tools in the future.
We propose a generalization of the widely used fractional Brownian motion (FBM), memory-multi-FBM (MMFBM), to describe viscoelastic or persistent anomalous diffusion with time-dependent memory exponent α(t ) in a changing environment. In MMFBM the built-in, long-range memory is continuously modulated by α(t ). We derive the essential statistical properties of MMFBM such as its response function, mean-squared displacement (MSD), autocovariance function, and Gaussian distribution. In contrast to existing forms of FBM with time-varying memory exponents but a reset memory structure, the instantaneous dynamic of MMFBM is influenced by the process history, e.g., we show that after a steplike change of α(t ) the scaling exponent of the MSD after the α step may be determined by the value of α(t ) before the change. MMFBM is a versatile and useful process for correlated physical systems with nonequilibrium initial conditions in a changing environment.
We present real-world data processing on measured electron time-of-flight data via neural networks. Specifically, the use of disentangled variational autoencoders on data from a diagnostic instrument for online wavelength monitoring at the free electron laser FLASH in Hamburg. Without a-priori knowledge the network is able to find representations of single-shot FEL spectra, which have a low signal-to-noise ratio. This reveals, in a directly human-interpretable way, crucial information about the photon properties. The central photon energy and the intensity as well as very detector-specific features are identified. The network is also capable of data cleaning, i.e. denoising, as well as the removal of artefacts. In the reconstruction, this allows for identification of signatures with very low intensity which are hardly recognisable in the raw data. In this particular case, the network enhances the quality of the diagnostic analysis at FLASH. However, this unsupervised method also has the potential to improve the analysis of other similar types of spectroscopy data.
In recurrence analysis, the tau-recurrence rate encodes the periods of the cycles of the underlying high-dimensional time series. It, thus, plays a similar role to the autocorrelation for scalar time-series in encoding temporal correlations.
However, its Fourier decomposition does not have a clean interpretation. Thus, there is no satisfactory analogue to the power spectrum in recurrence analysis.
We introduce a novel method to decompose the tau-recurrence rate using an over-complete basis of Dirac combs together with sparsity regularization.
We show that this decomposition, the inter-spike spectrum, naturally provides an analogue to the power spectrum for recurrence analysis in the sense that it reveals the dominant periodicities of the underlying time series.
We show that the inter-spike spectrum correctly identifies patterns and transitions in the underlying system in a wide variety of examples and is robust to measurement noise.
Gravitational waves emitted from the coalescence of neutron star binaries open a new window to probe matter and fundamental physics in unexplored, extreme regimes. To extract information about the supranuclear matter inside neutron stars and the properties of the compact binary systems, robust theoretical prescriptions are required. We give an overview about general features of the dynamics and the gravitational wave signal during the binary neutron star coalescence. We briefly describe existing analytical and numerical approaches to investigate the highly dynamical, strong-field region during the merger. We review existing waveform approximants and discuss properties and possible advantages and shortcomings of individual waveform models, and their application for real gravitational-wave data analysis.
Tropical cyclones range among the costliest of all meteorological events worldwide and planetary scale warming provides more energy and moisture to these storms. Modelling the national and global economic repercussions of 2017's Hurricane Harvey, we find a qualitative change in the global economic response in an increasingly warmer world.
While the United States were able to balance regional production failures by the original 2017 hurricane, this option becomes less viable under future warming.
In our simulations of over 7000 regional economic sectors with more than 1.8 million supply chain connections, the US are not able to offset the losses by use of national efforts with intensifying hurricanes under unabated warming.
At a certain warming level other countries have to step in to supply the necessary goods for production, which gives US economic sectors a competitive disadvantage. In the highly localized mining and quarrying sector-which here also comprises the oil and gas production industry-this disadvantage emerges already with the original Hurricane Harvey and intensifies under warming.
Eventually, also other regions reach their limit of what they can offset.
While we chose the example of a specific hurricane impacting a specific region, the mechanism is likely applicable to other climate-related events in other regions and other sectors.
It is thus likely that the regional economic sectors that are best adapted to climate change gain significant advantage over their competitors under future warming.
Diffusive search for a static target is a common problem in statistical physics with numerous applications in chemistry and biology.
We look at this problem from a different perspective and investigate the statistics of encounters between the diffusing particle and the target. While an exact solution of this problem was recently derived in the form of a spectral expansion over the eigenbasis of the Dirichlet-to-Neumann operator, the latter is generally difficult to access for an arbitrary target.
In this paper, we present three complementary approaches to approximate the probability density of the rescaled number of encounters with a small target in a bounded confining domain. In particular, we derive a simple fully explicit approximation, which depends only on a few geometric characteristics such as the surface area and the harmonic capacity of the target, and the volume of the confining domain.
We discuss the advantages and limitations of three approaches and check their accuracy.
We also deduce an explicit approximation for the distribution of the first-crossing time, at which the number of encounters exceeds a prescribed threshold. Its relations to common first-passage time problems are discussed.
First-passage times in conical varying-width channels biased by a transverse gravitational force
(2022)
We study the crossing time statistic of diffusing point particles between the two ends of expanding and narrowing two-dimensional conical channels under a transverse external gravitational field.
The theoretical expression for the mean first-passage time for such a system is derived under the assumption that the axial diffusion in a two-dimensional channel of smoothly varying geometry can be approximately described as a one-dimensional diffusion in an entropic potential with position-dependent effective diffusivity in terms of the modified Fick-Jacobs equation.
We analyze the channel crossing dynamics in terms of the mean first-passage time, combining our analytical results with extensive two-dimensional Brownian dynamics simulations, allowing us to find the range of applicability of the one-dimensional approximation.
We find that the effective particle diffusivity decreases with increasing amplitude of the external potential.
Remarkably, the mean first-passage time for crossing the channel is shown to assume a minimum at finite values of the potential amplitude.
It is often claimed that the entropy of a network's degree distribution is a proxy for its robustness. Here, we clarify the link between degree distribution entropy and giant component robustness to node removal by showing that the former merely sets a lower bound to the latter for randomly configured networks when no other network characteristics are specified. Furthermore, we show that, for networks of fixed expected degree that follow degree distributions of the same form, the degree distribution entropy is not indicative of robustness. By contrast, we show that the remaining degree entropy and robustness have a positive monotonic relationship and give an analytic expression for the remaining degree entropy of the log-normal distribution. We also show that degree-degree correlations are not by themselves indicative of a network's robustness for real networks. We propose an adjustment to how mutual information is measured which better encapsulates structural properties related to robustness.
We discuss the coherent splitting and recombining of a nanoparticle in a mesoscopic "closed-loop" Stern-Gerlach interferometer in which the observable is the spin of a single impurity embedded in the particle.
This spin, when interacting with a pulsed magnetic gradient, generates the force on the particle.
We calculate the internal decoherence, which arises as the displaced impurity excites internal degrees of freedom (phonons) that may provide WelcherWeg information and preclude interference.
We estimate the constraints this decoherence channel puts on future interference experiments with massive objects. We find that for a wide range of masses, forces, and temperatures, phonons do not inhibit Stern-Gerlach interferometry with micro-scale objects.
However, phonons do constitute a fundamental limit on the splitting of larger macroscopic objects if the applied force induces phonons.
The radiation model is a parameter-free model of human mobility that has been applied primarily for short-distance moves, such as commuting. When applied to migration, it underestimates the number of long-range moves, such as between different US states. Here we show that it additionally suffers from a conceptual inconsistency that can have substantial numerical effects on long-distance moves.
We propose a modification of the radiation model that introduces a dependence on the angle between any two alternative potential destinations, accounting for the possibility that migrants may have preferences about the approximate direction of their move.
We demonstrate that this modification mitigates the conceptual inconsistency and improves the model fit to observational migration data, without introducing any fitting parameters.
Contour scanning and process gas type are process parameters typically considered achieving second order effects compared to first order factors such as laser power and scanning speed.
The present work highlights that contour scanning is crucial to ensure geometrical accuracy and thereby the high performance under uniaxial compression of complex Alloy 718 lattice structures.
Studies of X-ray computed tomography visualizations of as-built and compression-strained structures reveal the continuous and smooth bending and compression of the walls, and the earlier onset of internal contact appearance in the denser lattices printed with contour. In contrast, the effect of addition of He to the Ar process gas appears to have limited influence on the mechanical response of the lattices and their microstructure as characterized by electron backscattered diffraction.
However, the addition of He proved to significantly enhance the cooling rate and to reduce the amount of the generated spatters as evidenced by in situ monitoring of the process emissions, which is very promising for the process stability and powder reusability during laser powder bed fusion.
In this work, we investigate the photo-aquation reaction of the ferrocyanide anion with multi-edge picosecond soft X-ray spectroscopy.
Combining the information of the iron L-edge with nitrogen and oxygen K-edges, we carry out a complete characterization of the bonding channels in the [Fe(CN)(5)(H2O)](3-) photo-product.
We observe clear spectral signatures of covalent bonding between water and the metal, reflecting the mixing of the Fe d(z)(2) orbital with the 3a(1) and 4a(1) orbitals of H2O. Additional fingerprints related to the symmetry reduction and the resulting loss in orbital degeneracy are also reported.
The implications of the elucidated fingerprints in the context of future ultra-fast experiments are also discussed.
In the Universe, matter outside of stars and compact objects is mostly composed of collisionless plasma.
The interaction of a supersonic plasma flow with an obstacle results in collisionless shocks that are often associated with intense nonthermal radiation and the production of cosmic ray particles.
Motivated by simulations of non-relativistic high-Mach-number shocks in supernova remnants, we investigate the instabilities excited by relativistic electron beams in the extended foreshock of oblique shocks.
The phase-space distributions in the inner and outer foreshock regions are derived with a particle-in-cell simulation of the shock and used as initial conditions for simulations with periodic boundary conditions to study their relaxation toward equilibrium.
We find that the observed electron-beam instabilities agree very well with the predictions of a linear dispersion analysis: the electrostatic electron-acoustic instability dominates in the outer region of the foreshock, while the denser electron beams in the inner foreshock drive the gyroresonant oblique-whistler instability.
Ground-based solar observations are severely affected by Earth's turbulent atmosphere. As a consequence, observed image quality and prevailing seeing conditions are closely related. Partial correction of image degradation is nowadays provided in real time by adaptive optics (AO) systems. In this study, different metrics of image quality are compared with parameters characterizing the prevailing seeing conditions, i.e. Median Filter Gradient Similarity (MFGS), Median Filter Laplacian Similarity (MFLS), Helmli-Scherer mean, granular rms-contrast, differential image motion, and Fried-parameter r(0). The quiet-Sun observations at disk center were carried out at the Vacuum Tower Telescope (VTT), Observatorio del Teide (OT), Izana, Tenerife, Spain. In July and August 2016, time series of short-exposure images were recorded with the High-resolution Fast Imager (HiFI) at various wavelengths in the visible and near-infrared parts of the spectrum. Correlation analysis yields the wavelength dependence of the image quality metrics and seeing parameters, and Uniform Manifold Approximation and Projection (UMAP) is employed to characterize the seeing on a particular observing day. In addition, the image quality metrics and seeing parameters are used to determine the field dependence of the correction provided by the AO system. Management of high-resolution imaging data from large-aperture, ground-based telescopes demands reliable image quality metrics and meaningful characterization of prevailing seeing conditions and AO performance. The present study offers guidance on how retrieving such information ex post facto.
Self-organized patterns in the actin cytoskeleton are essential for eukaryotic cellular life. They are the building blocks of many functional structures that often operate simultaneously to facilitate, for example, nutrient uptake and movement of cells. However, identifying how qualitatively distinct actin patterns can coexist remains a challenge.
Using bifurcation theory of a mass conserved activator-inhibitor system, we uncover a generic mechanism of how different actin waves-traveling waves and excitable pulses- organize and simultaneously emerge.
Live-cell imaging experiments indeed reveal that narrow, planar, and fast-moving excitable pulses may coexist with ring-shaped macropinocytic actin waves in the cortex of motile amoeboid cells.
This joint experimental-theoretical work focuses on molecular and photophysical properties of the spiropyran-containing amphiphilic molecule in organic and aqueous solutions.
Being dissolved in tested organic solvents, the system demonstrates positive photochromism, i.e., upon UV stimulus the colorless spiropyran form is transformed into colorful merocyanine isomer.
However, the aqueous solution of the amphiphile possesses a negative photochromism: the orange-red merocyanine form becomes thermodynamically more stable in water, and both UV and vis stimuli lead to the partial or complete photobleaching of the solution.
The explanation of this phenomenon is given on the basis of density functional theory calculations and classical modeling including thermodynamic integration.
The simulations reveal that stabilization of merocyanine in water proceeds with the energy of ca. 70 kJ mol-1, and that the Helmholtz free energy of hydration of merocyanine form is 100 kJ mol-1 lower as compared to the behavior of SP isomer in water.
The explanation of such a difference lies in the molecular properties of the merocyanine: after ring-opening reaction this molecule transforms into a zwitterionic form, as evidenced by the electrostatic potential plotted around the opened form.
The presence of three charged groups on the periphery of a flat conjugated backbone stimulates the self-assembly of merocyanine molecules in water, ending up with the formation of elongated associates with stack-like building blocks, as shown in molecular dynamics simulations of the aqueous solution with the concentration above critical micelle concentration.
Our quantitative evaluation of the hydrophilicity switching in spiropyran/merocyanine containing surfactants may prompt the search for new systems, including colloidal and polymeric ones, aiming at remote tuning of their morphology, which could give new promising shapes and patterns for the needs of modern nanotechnology.
Carbon suboxide (C3O2) is a unique molecule able to polymerize spontaneously into highly conjugated light-absorbing structures at temperatures as low as 0 degrees C. Despite obvious advantages, little is known about the nature and the functional properties of this carbonaceous material. In this work, the aim is to bring "red carbon," a forgotten polymeric semiconductor, back to the community's attention.
A solution polymerization process is adapted to simplify the synthesis and control the structure.
This allows one to obtain this crystalline covalent material at low temperatures. Both spectroscopic and elemental analyses support the chemical structure represented as conjugated ladder polypyrone ribbons.
Density functional theory calculations suggest a crystalline structure of AB stacks of polypyrone ribbons and identify the material as a direct bandgap semiconductor with a medium bandgap that is further confirmed by optical analysis.
The material shows promising photocatalytic performance using blue light.
Moreover, the simple condensation-aromatization route described here allows the straightforward fabrication of conjugated ladder polymers and can be inspiring for the synthesis of carbonaceous materials at low temperatures in general.
In this paper, we propose a revised fractional Brownian motion run with a nonlinear clock (fBm-nlc) model and utilize it to illustrate the microscopic mechanism analysis of the fractal derivative diffusion model with variable coefficient (VC-FDM).
The power-law mean squared displacement (MSD) links the fBm-nlc model and the VC-FDM via the two-parameter power law clock and the Hurst exponent is 0.5.
The MSD is verified by using the experimental points of the chloride ions diffusion in concrete.
When compared to the linear Brownian motion, the results show that the power law MSD of the fBm-nlc is much better in fitting the experimental points of chloride ions in concrete.
The fBm-nlc clearly interprets the VC-FDM and provides a microscopic strategy in characterizing different types of non-Fickian diffusion processes with more different nonlinear functions.
The printability of artificial defects inside the additively manufactured laser powder bed fusion (LPBF) 316L stainless steel is investigated.
The printing parameters of the LPBF process are optimized to produce artificial defects with reproducible sizes at desired positions while minimizing redundant porosity. The smallest obtained artificial defect is 90 mu m in diameter.
The accuracy of the geometry of the printed defect depends on both the height and the diameter in the input model.
The effect of artificial defects on the very-high-cycle fatigue (VHCF) behavior of LPBF 316L stainless steel is also studied. The specimens printed with artificial defects in the center are tested under VHCF using an ultrasonic machine.
Crack initiation is accompanied by the formation of a fine granular area (FGA), typical of VHCF. Despite the presence of relatively large artificial defects, FGA formation is observed around accidental natural printing defects closer to the surface, which can still be considered as internal. The causes for this occurrence are discussed.
As society paves its way towards device miniaturization and precision medicine, microscale actuation and transport become increasingly prominent research fields with high impact in both technological and clinical contexts.
In order to accomplish movement of micron-sized objects towards specific target sites, active biohybrid transport systems, such as motile living cells that act as smart biochemically powered microcarriers, have been suggested as an alternative to synthetic microrobots.
Inspired by the motility of leukocytes, we propose the amoeboid crawling of eukaryotic cells as a promising mechanism for transport of micron-sized cargoes and present an in-depth study of this type of composite active matter.
Its transport properties result from the interactions of an active element (cell) and a passive one (cargo) and reveal an optimal cargo size that enhances the locomotion of the load-carrying cells, even exceeding their motility in the absence of cargo.
The experimental findings are rationalized in terms of a biohybrid active particle model that describes the emergent cell-cargo dynamics and enables us to derive the long-time diffusive transport of amoeboid microcarriers.
As amoeboid locomotion is commonly observed for mammalian cells such as leukocytes, our results lay the foundations for the study of transport performance of other medically relevant cell types and for extending our findings to more advanced transport tasks in complex environments, such as tissues.
Hybrid nanophotonic elements, fabricated by organic and inorganic materials, are going to be key components of modern devices.
Coupled systems of photoemitters with a plasmonic waveguide serve the demand for nanoscopic frequency converters.
However, processes like the degradation of the photoemitters via photobleaching occur and need to be monitored and controlled, to realize future successful devices.
We introduce a hybrid perylene-diimide / silver nanowire as plasmon frequency converter. A versatile method is presented to monitor and analyze the bleaching process. It is based on a time series of photoluminescence images, during the operation of a single converter.
An analytical model is applied on the data and unveils that the photobleaching rate is constant and independent of the operation of the plasmon converter.
We have investigated the self-assembly of the graphene nanoribbon molecular precursor 10,10'-dibromo-9,9'-bianthryl (DBBA) on Au(111) with frequency modulation scanning force microscopy (FM-SFM) at room temperature combined with ab initio calculations.
For low molecular coverages, the molecules aggregate along the substrate herringbone reconstruction main directions while remaining mobile.
At intermediate coverage, two phases coexist, zigzag stripes of monomer chains and decorated herringbones. For high coverage, the molecules assemble in a dimer-striped phase.
The adsorption behaviour of DBBA molecules and their interactions are discussed and compared with the results from ab initio calculations.
The diffusion process of water in swelling (expansive) soil often deviates from normal Fick diffusion and belongs to anomalous diffusion.
The process of water adsorption by swelling soil often changes with time, in which the microstructure evolves with time and the absorption rate changes along a fractal dimension gradient function.
Thus, based on the material coordinate theory, this paper proposes a variable order derivative fractal model to describe the cumulative adsorption of water in the expansive soil, and the variable order is time dependent linearly.
The cumulative adsorption is a power law function of the anomalous sorptivity, and patterns of the variable order.
The variable-order fractal derivative model is tested to describe the cumulative adsorption in chernozemic surface soil, Wunnamurra clay and sandy loam.
The results show that the fractal derivative model with linearly time dependent variable-order has much better accuracy than the fractal derivative model with a constant derivative order and the integer order model in the application cases.
The derivative order can be used to distinguish the evolution of the anomalous adsorption process. The variable-order fractal derivative model can serve as an alternative approach to describe water anomalous adsorption in swelling soil.
Time and angle-resolved time-of-flight electron spectroscopy for functional materials science
(2022)
Electron spectroscopy with the unprecedented transmission of angle-resolved time-of-flight detection, in combination with pulsed X-ray sources, brings new impetus to functional materials science.
We showcase recent developments towards chemical sensitivity from electron spectroscopy for chemical analysis and structural information from photoelectron diffraction using the phase transition properties of 1T-TaS2.
Our development platform is the SurfaceDynamics instrument located at the Femtoslicing facility at BESSY II, where femtosecond and picosecond X-ray pulses can be generated and extracted.
The scientific potential is put into perspective to the current rapidly developing pulsed X-ray source capabilities from Lasers and Free-Electron Lasers.
Current evidence suggests that migratory animals extract map information from the geomagnetic field for true navigation. The sensory basis underlying this feat is elusive, but presumably involves magnetic particles.
A common experimental manipulation procedure consists of pre-treating animals with a magnetic pulse, with the aim of re-magnetising particles to alter the internal representation of the external field prior to a navigation task.
Although pulsing provoked deflected bearings in caged songbirds, analogous studies with free-flying songbirds yielded inconsistent results.
Here, we pulsed European robins (Erithacus rubecula) at an offshore stopover site during spring migration and monitored their free-flight behaviour with a regional-scale network of radio-receiving stations.
We found no pulse effect on departure probability, nocturnal departure timing departure direction or consistency of flight direction.
This suggests either no use of the geomagnetic map by our birds, or that magnetic pulses do not affect the sensory system underlying geomagnetic map detection.
In this work we present windlidar data for the research village Ny-Alesund located on Svalbard in the European Arctic (78.923 degrees N, 11.928 degrees F) from 2013 to 2021.
The data have a resolution of 50 m and 10 min with an overlapping height of about 150 m.
The maximum range depends on the meteorologic situation. Up to 1000 m altitude the data availability is better than 71%.
We found that the highest wind speeds occur in November and December, the lowest ones in June and July, up to 500 m altitude the wind is channelled strongly in ESE to NW direction parallel to the fjord axis and the synoptic conditions above 1000 m altitude already dominate.
While the fraction of windy days (v > 10 m/s) varies significantly from month to month, there is no overall trend of the wind visible in our data set.
We define gusts and jets by the requirement of wind maxima v > 2 m/s above and below a wind maximum. In total, more than 24,000 of these events were identified (corresponding to 6% of the time), of which 223 lasted for at least 100 min ("Long Jets"). All of these events are fairly equally distributed over the months relatively to the available data.
Further, gusts and jets follow different distributions (in terms of altitude or depths) and occur more frequently for synoptic flow from roughly a southerly direction. Jets do not show a clear correlation between occurrence and synoptic flow. Gusts and jets are not related to cloud cover.
We conclude that the atmosphere from 400 m to 1000 m above Ny-Alesund is dominated by a turbulent wind shear zone, which connects the micrometeorology in the atmospheric boundary layer (ABL) with the synoptic flow.
This international curricular review provides a structured overview of the particle physics content in 27 state, national, and international high-school physics curricula. The review was based on a coding manual that included 60 concepts that were identified as relevant for high-school particle physics education.
Two types of curricula were reviewed, namely curricula with a dedicated particle physics chapter and curricula without a dedicated particle physics chapter.
The results of the curricular review show that particle physics concepts are explicitly or implicitly present in all reviewed curricula.
However, the number of particle physics concepts that are featured in a curriculum varies greatly across the reviewed curricula. We identified core particle physics concepts that can be found in most curricula. Here, elementary particles, fundamental interactions, and charges were identified as explicit particle physics concepts that are featured in more than half of the reviewed curricula either as content or context. Indeed, theoretical particle physics concepts are more prominent in high-school physics curricula than experimental particle physics concepts.
Overall, this international curricular review provides the basis for future curricular development with respect to particle physics and suggests an increased inclusion of experimental particle physics concepts in high-school physics curricula.
The work is devoted to the use of electrokinetic phenomena in liquid crystals to create a new class of microfluidics devices - optofluidics, designed to control electromagnetic radiation, including the THz frequency range.
To achieve the goal, an optical method is used to study changes in the orientational structure in LC layers caused by a shear flow generated by electroosmotic pumps. Simula-tion of LC behaviour in an experimental cell containing electroosmotic pumps and flat layers of a nematic liquid crystal is fulfilled.
The experimental depend-ences of the intensity of polarized radiation passing through flat LC layers on the control voltage applied to the electroosmotic pump and the results of calcu-lations of the hydrodynamic and mechano-optical characteristics of the experi-mental LC cell are presented.
The propagation of THz irradiation across the multilayer structure of the optofluidic cell is considered taking into account the minimum number of re-reflections of waves from different layers and the ab-sorption of THz irradiation in a propylene and a liquid crystal.
We report on the effect of spatially correlated noise on the velocities of self-propelled particles.
Correlations in the random forces acting on self-propelled particles can induce directed collective motion, i.e., swarming.
Even with repulsive coupling in the velocity directions, which favors a disordered state, strong correlations in the fluctuations can align the velocities locally leading to a macroscopic, turbulent velocity field.
On the other hand, while spatially correlated noise is aligning the velocities locally, the swarming transition to globally directed motion is inhibited when the correlation length of the noise is nonzero, but smaller than the system size.
We analyze the swarming transition in d-dimensional space in a mean field model of globally coupled velocity vectors.
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.
In the soil bacterium Pseudomonas putida, the motor torque for flagellar rotation is generated by the two stators MotAB and MotCD.
Here, we construct mutant strains in which one or both stators are knocked out and investigate their swimming motility in fluids of different viscosity and in heterogeneous structured environments (semisolid agar).
Besides phase-contrast imaging of single-cell trajectories and spreading cultures, dual-color fluorescence microscopy allows us to quantify the role of the stators in enabling P. putida's three different swimming modes, where the flagellar bundle pushes, pulls, or wraps around the cell body.
The MotAB stator is essential for swimming motility in liquids, while spreading in semisolid agar is not affected. Moreover, if the MotAB stator is knocked out, wrapped mode formation under low-viscosity conditions is strongly impaired and only partly restored for increased viscosity and in semisolid agar.
In contrast, when the MotCD stator is missing, cells are indistinguishable from the wild type in fluid experiments but spread much more slowly in semisolid agar.
Analysis of the microscopic trajectories reveals that the MotCD knockout strain forms sessile clusters, thereby reducing the number of motile cells, while the swimming speed is unaffected. Together, both stators ensure a robust wild type that swims efficiently under different environmental conditions.
IMPORTANCE
Because of its heterogeneous habitat, the soil bacterium Pseudomonas putida needs to swim efficiently under very different environmental conditions. In this paper, we knocked out the stators MotAB and MotCD to investigate their impact on the swimming motility of P. putida.
While the MotAB stator is crucial for swimming in fluids, in semisolid agar, both stators are sufficient to sustain a fast-swimming phenotype and increased frequencies of the wrapped mode, which is known to be beneficial for escaping mechanical traps. However, in contrast to the MotAB knockout, a culture of MotCD knockout cells spreads much more slowly in the agar, as it forms nonmotile clusters that reduce the number of motile cells.
Because of its heterogeneous habitat, the soil bacterium Pseudomonas putida needs to swim efficiently under very different environmental conditions. In this paper, we knocked out the stators MotAB and MotCD to investigate their impact on the swimming motility of P. putida.
The quantification and identification of aerosols in industry plays a key role in process monitoring and control and lays the foundation for process automation aspired by the industry 4.0 initiative.
However, measuring particulate matter's mass and number concentrations in harsh environments poses great analytical constraints.
The presented approach comprises a comprehensive set of light-and imaging-based techniques, all contactless, in-line, and real-time. It includes, but is not limited to, stroboscopic imaging, laser-induced breakdown spectroscopy (LIBS) and laser-induced incandescence (LII). Stroboscopic imaging confirmed the particles sphericity and was used to measure the particle number density. A phase-selective LIBS setup with low fluence and 500 Hz repetition rate was used to classify each particle with a single-pulse and in real time. Simultaneously, the created plasma was captured by CCD imaging to determine the detection volume and hit rate of the LIBS setup.
Both data sets combined were converted to a particle number density, which was consistent with the particle number density of the stroboscopic measurements. Furthermore, using a photodiode and microphone in parallel to the LIBS setup allowed for the photoacoustic normalization of the spectral line intensity at the laser repetition rate of 500 Hz.
This was done as a partial photoacoustic normalization method with the cut-off based on the coefficient of variation (CV), reducing it by 25%. Aside from that photodiode and microphone were proven to be valuable event counting with the advantage of the less spatially constricted. A second laser setup was used for laser -induced incandescence (LII) making it possible to classify the particles based on their incandescence tendency. Given its larger probing volume, LII could be employed at very low particle number densities.
With respect to the current literature, this is the first approach of using LII as an in-line, real-time analytical technique for the compositional classification of metal-bearing aerosols.
The BAMline at the BESSY II synchrotron X-ray source has enabled research for more than 20 years in widely spread research fields such as materials science, biology, cultural heritage and medicine.
As a nondestructive characterization method, synchrotron X-ray imaging, especially tomography, plays a particularly important role in structural characterization.
A recent upgrade of key equipment of the BAMline widens its imaging capabilities: shorter scan acquisition times are now possible, in situ and op erando studies can now be routinely performed, and different energy spectra can easily be set up.
In fact, the upgraded double-multilayer monochromator brings full flexibility by yielding different energy spectra to optimize flux and energy resolution as desired.
The upgraded detector (based on an sCMOS camera) also allows exploiting the higher flux with reduced readout times.
Furthermore, an installed slip ring allows the sample stage to continuously rotate.
The latter feature enables tomographic observation of processes occurring in the time scale of a few seconds.
Inferring oscillator's phase and amplitude response from a scalar signal exploiting test stimulation
(2022)
The phase sensitivity curve or phase response curve (PRC) quantifies the oscillator's reaction to stimulation at a specific phase and is a primary characteristic of a self-sustained oscillatory unit.
Knowledge of this curve yields a phase dynamics description of the oscillator for arbitrary weak forcing. Similar, though much less studied characteristic, is the amplitude response that can be defined either using an ad hoc approach to amplitude estimation or via the isostable variables.
Here, we discuss the problem of the phase and amplitude response inference from observations using test stimulation. Although PRC determination for noise-free neuronal-like oscillators perturbed by narrow pulses is a well-known task, the general case remains a challenging problem. Even more challenging is the inference of the amplitude response. This characteristic is crucial, e.g. for controlling the amplitude of the collective mode in a network of interacting units-a task relevant to neuroscience. Here, we compare the performance of different techniques suitable for inferring the phase and amplitude response, particularly with application to macroscopic oscillators. We suggest improvements to these techniques, e.g. demonstrating how to obtain the PRC in case of stimuli of arbitrary shape. Our main result is a novel technique denoted by IPID-1, based on the direct reconstruction of the Winfree equation and the analogous first-order equation for isostable dynamics. The technique works for signals with or without well-pronounced marker events and pulses of arbitrary shape; in particular, we consider charge-balanced pulses typical in neuroscience applications. Moreover, this technique is superior for noisy and high-dimensional systems. Additionally, we describe an error measure that can be computed solely from data and complements any inference technique.
Random logic networks
(2021)
We investigate dynamical properties of a quantum generalization of classical reversible Boolean networks. The state of each node is encoded as a single qubit, and classical Boolean logic operations are supplemented by controlled bit-flip and Hadamard operations. We consider synchronous updating schemes in which each qubit is updated at each step based on stored values of the qubits from the previous step. We investigate the periodic or quasiperiodic behavior of quantum networks, and we analyze the propagation of single site perturbations through the quantum networks with input degree one. A nonclassical mechanism for perturbation propagation leads to substantially different evolution of the Hamming distance between the original and perturbed states.
We apply the concepts of relative dimensions and mutual singularities to characterize the fractal properties of overlapping attractor and repeller in chaotic dynamical systems. We consider one analytically solvable example (a generalized baker's map); two other examples, the Anosov-Mobius and the Chirikov-Mobius maps, which possess fractal attractor and repeller on a two-dimensional torus, are explored numerically. We demonstrate that although for these maps the stable and unstable directions are not orthogonal to each other, the relative Renyi and Kullback-Leibler dimensions as well as the mutual singularity spectra for the attractor and repeller can be well approximated under orthogonality assumption of two fractals.
The fundamental sensitivity limit of atomic force microscopy is strongly correlated to the thermal noise of cantilever oscillation. A method to suppress this unwanted noise is to reduce the bandwidth of the measurement, but this approach is limited by the speed of the measurement and the width of the cantilever resonance, commonly defined through the quality factor Q. However, it has been shown that optomechanical resonances in interferometers might affect cantilever oscillations resulting in an effective quality factor Q(eff). When the laser power is sufficiently increased cantilever oscillations might even reach the regime of self-oscillation. In this self-oscillation state, the noise of the system is partially determined by the interaction with laser light far from equilibrium. Here, we show and discuss how tuning of laser power leads to nonlinear optomechanical effects that can dramatically increase the effective quality factor of the cantilever leading to out-of-equilibrium noise. We model the effects using a fourth order nonlinearity of the damping coefficient. Published under an exclusive license by AIP Publishing.
Data-driven expectations for electromagnetic counterpart searches based on LIGO/Virgo public alerts
(2022)
Searches for electromagnetic counterparts of gravitational-wave signals have redoubled since the first detection in 2017 of a binary neutron star merger with a gamma-ray burst, optical/infrared kilonova, and panchromatic afterglow. Yet, one LIGO/Virgo observing run later, there has not yet been a second, secure identification of an electromagnetic counterpart. This is not surprising given that the localization uncertainties of events in LIGO and Virgo's third observing run, O3, were much larger than predicted.
We explain this by showing that improvements in data analysis that now allow LIGO/Virgo to detect weaker and hence more poorly localized events have increased the overall number of detections, of which well-localized, gold-plated events make up a smaller proportion overall.
We present simulations of the next two LIGO/Virgo/KAGRA observing runs, O4 and O5, that are grounded in the statistics of O3 public alerts. To illustrate the significant impact that the updated predictions can have, we study the follow-up strategy for the Zwicky Transient Facility. Realistic and timely forecasting of gravitational-wave localization accuracy is paramount given the large commitments of telescope time and the need to prioritize which events are followed up.
We include a data release of our simulated localizations as a public proposal planning resource for astronomers.
Stochastic resetting, a diffusive process whose amplitude is reset to the origin at random times, is a vividly studied strategy to optimize encounter dynamics, e.g., in chemical reactions. Here we generalize the resetting step by introducing a random resetting amplitude such that the diffusing particle may be only partially reset towards the trajectory origin or even overshoot the origin in a resetting step. We introduce different scenarios for the random-amplitude stochastic resetting process and discuss the resulting dynamics. Direct applications are geophysical layering (stratigraphy) and population dynamics or financial markets, as well as generic search processes.
Comb-like geometric constraints leading to emergence of the time-fractional Schrödinger equation
(2021)
This paper presents an overview over several examples, where the comb-like geometric constraints lead to emergence of the time-fractional Schrodinger equation. Motion of a quantum object on a comb structure is modeled by a suitable modification of the kinetic energy operator, obtained by insertion of the Dirac delta function in the Laplacian. First, we consider motion of a free particle on two- and three-dimensional comb structures, and then we extend the study to the interacting cases. A general form of a nonlocal term, which describes the interactions of the particle with the medium, is included in the Hamiltonian, and later on, the cases of constant and Dirac delta potentials are analyzed. At the end, we discuss the case of non-integer dimensions, considering separately the case of fractal dimension between one and two, and the case of fractal dimension between two and three. All these examples show that even though we are starting with the standard time-dependent Schrodinger equation on a comb, the time-fractional equation for the Green's functions appears, due to these specific geometric constraints.