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Monolithic perovskite silicon tandem solar cells can overcome the theoretical efficiency limit of silicon solar cells. This requires an optimum bandgap, high quantum efficiency, and high stability of the perovskite. Herein, a silicon heterojunction bottom cell is combined with a perovskite top cell, with an optimum bandgap of 1.68 eV in planar p-i-n tandem configuration. A methylammonium-free FA(0.75)Cs(0.25)Pb(I0.8Br0.2)(3) perovskite with high Cs content is investigated for improved stability. A 10% molarity increase to 1.1 m of the perovskite precursor solution results in approximate to 75 nm thicker absorber layers and 0.7 mA cm(-2) higher short-circuit current density. With the optimized absorber, tandem devices reach a high fill factor of 80% and up to 25.1% certified efficiency. The unencapsulated tandem device shows an efficiency improvement of 2.3% (absolute) over 5 months, showing the robustness of the absorber against degradation. Moreover, a photoluminescence quantum yield analysis reveals that with adapted charge transport materials and surface passivation, along with improved antireflection measures, the high bandgap perovskite absorber has the potential for 30% tandem efficiency in the near future.
We discuss an efficient Hierarchical Effective Mode (HEM) representation of a high-dimensional harmonic oscillator bath, which describes phonon-driven vibrational relaxation of an adsorbate-surface system, namely, deuterium adsorbed on Si(100). Starting from the original Hamiltonian of the adsorbate-surface system, the HEM representation is constructed via iterative orthogonal transformations, which are efficiently implemented with Householder matrices. The detailed description of the HEM representation and its construction are given in the second quantization representation. The hierarchical nature of this representation allows access to the exact quantum dynamics of the adsorbate-surface system over finite time intervals, controllable via the truncation order of the hierarchy. To study the convergence properties of the effective mode representation, we solve the time-dependent Schrodinger equation of the truncated system-bath HEM Hamiltonian, with the help of the multilayer extension of the Multiconfigurational Time-Dependent Hartree (ML-MCTDH) method. The results of the HEM representation are compared with those obtained with a quantum-mechanical tier-model. The convergence of the HEM representation with respect to the truncation order of the hierarchy is discussed for different initial conditions of the adsorbate-surface system. The combination of the HEM representation with the ML-MCTDH method provides information on the time evolution of the system (adsorbate) and multiple effective modes of the bath (surface). This permits insight into mechanisms of vibration-phonon coupling of the adsorbate-surface system, as well as inter-mode couplings of the effective bath.
Here, a promising approach for producing piezo-polymer transducers in a one-step process is presented. Using 3D-printing technology and polypropylene (PP) filaments, we are able to print a two-layered film structure with regular cavities of precisely controlled size and shape. It is found that the 3D-printed samples exhibit piezoelectric coefficients up to 200 pC/N, similar to those of other PP ferroelectrets, and their temporal and thermal behavior is in good agreement with those known of PP ferroelectrets. The piezoelectric response strongly decreases for applied pressures above 20 kPa, as the pressure in the air-filled cavities strongly influences the overall elastic modulus of ferroelectrets.
Motivated by the observation of non-exponential run-time distributions of bacterial swimmers, we propose a minimal phenomenological model for taxis of active particles whose motion is controlled by an internal clock. The ticking of the clock depends on an external concentration field, e.g., a chemical substance. We demonstrate that these particles can detect concentration gradients and respond to them by moving up- or down-gradient depending on the clock design, albeit measurements of these fields are purely local in space and instantaneous in time. Altogether, our results open a new route in the study of directional navigation: we show that the use of a clock to control motility actions represents a generic and versatile toolbox to engineer behavioral responses to external cues, such as light, chemical, or temperature gradients.
A novel design of an electrochemical anodization cell dedicated to the synthesis of mesoporous, single-crystalline silicon is presented. First and foremost, the design principle follows user safety since electrochemical etching of silicon requires highly hazardous electrolytes based on hydrofluoric (HF) acid. The novel cell design allows for safe electrolyte handling prior, during, and post-etching. A peristaltic pump with HF-resistant fluoroelastomer tubing transfers electrolytes between dedicated reservoirs and the anodization cell. Due to the flexibility of the cell operation, different processing conditions can be realized providing a large parameter range for the attainable sample thickness, its porosity, and the mean pore size. Rapid etching on the order of several minutes to synthesize micrometer-thick porous silicon epilayers on bulk silicon is possible as well as long-time etching with continuous, controlled electrolyte flow for several days to prepare up to 1000 mu m thick self-supporting porous silicon membranes. A highly adaptable, LabVIEW((TM))-based control software allows for user-defined etching profiles.
Whereas self-propelled hard discs undergo motility-induced phase separation, self-propelled rods exhibit a variety of nonequilibrium phenomena, including clustering, collective motion, and spatio-temporal chaos. In this work, we present a theoretical framework representing active particles by continuum fields. This concept combines the simplicity of alignment-based models, enabling analytical studies, and realistic models that incorporate the shape of self-propelled objects explicitly. By varying particle shape from circular to ellipsoidal, we show how nonequilibrium stresses acting among self-propelled rods destabilize motility-induced phase separation and facilitate orientational ordering, thereby connecting the realms of scalar and vectorial active matter. Though the interaction potential is strictly apolar, both, polar and nematic order may emerge and even coexist. Accordingly, the symmetry of ordered states is a dynamical property in active matter. The presented framework may represent various systems including bacterial colonies, cytoskeletal extracts, or shaken granular media. Interacting self-propelled particles exhibit phase separation or collective motion depending on particle shape. A unified theory connecting these paradigms represents a major challenge in active matter, which the authors address here by modeling active particles as continuum fields.
We consider a perturbation of the de Rham complex on a compact manifold with boundary. This perturbation goes beyond the framework of complexes, and so cohomology does not apply to it. On the other hand, its curvature is "small", hence there is a natural way to introduce an Euler characteristic and develop a Lefschetz theory for the perturbation. This work is intended as an attempt to develop a cohomology theory for arbitrary sequences of linear mappings.
Subdwarf B stars are core-helium-burning stars located on the extreme horizontal branch (EHB). Extensive mass loss on the red giant branch is necessary to form them. It has been proposed that substellar companions could lead to the required mass loss when they are engulfed in the envelope of the red giant star. J08205+0008 was the first example of a hot subdwarf star with a close, substellar companion candidate to be found. Here, we perform an in-depth re-analysis of this important system with much higher quality data allowing additional analysis methods. From the higher resolution spectra obtained with ESO-VLT/XSHOOTER, we derive the chemical abundances of the hot subdwarf as well as its rotational velocity. Using the Gaia parallax and a fit to the spectral energy distribution in the secondary eclipse, tight constraints to the radius of the hot subdwarf are derived. From a long-term photometric campaign, we detected a significant period decrease of -3.2(8) x 10(-12) dd(-1). This can be explained by the non-synchronized hot subdwarf star being spun up by tidal interactions forcing it to become synchronized. From the rate of period decrease we could derive the synchronization time-scale to be 4 Myr, much smaller than the lifetime on EHB. By combining all different methods, we could constrain the hot subdwarf to a mass of 0.39-0.50 M-circle dot and a radius of R-sdB = 0.194 +/- 0.008 R-circle dot, and the companion to 0.061-0.071 M-circle dot with a radius of R-comp = 0.092 +/- 0.005 R-circle dot, below the hydrogen-burning limit. We therefore confirm that the companion is most likely a massive brown dwarf.
For hybrid organic-inorganic as well as all-inorganic lead halide perovskites a Rashba effect has been invoked to explain the high efficiency in energy conversion by prohibiting direct recombination. Both a bulk and surface Rashba effect have been predicted. In the valence band of methylammonium (MA) lead bromide a Rashba effect has been reported by angle-resolved photoemission and circular dichroism with giant values of 7-11 eV angstrom. We present band dispersion measurements of MAPbBr(3) and spin-resolved photoemission of CsPbBr3 to show that a large Rashba effect detectable by photoemission or circular dichroism does not exist and cannot be the origin of the high effciency.
We report on the adsorption kinetics of azoben-zene-containing surfactants on solid surfaces of different hydrophobicity. The understanding of this processes is of great importance for many interfacial phenomena that can be actuated and triggered by light, since the surfactant molecules contain a photoresponsive azobenzene group in their hydrophobic tail. Three surfactant types are studied, differing in the spacer connecting the headgroup and the azobenzene unit by between 6 and 10 CH2 groups. Under irradiation with light of a suitable wavelength, the azobenzene undergoes reversible photoisomerization between two states, a nonpolar trans-state and a highly polar cis-state. Consequently, the surfactant molecule changes its hydrophobicity and thus affinity to a surface depending on the photoisomerization state of the azobenzene. The adsorption behavior on hydrophilic (glass) and hydrophobic (TeflonAF) surfaces is analyzed using quartz crystal microbalance with dissipation (QCM-D) and zeta-potential measurements. At equilibrium, the adsorbed surfactant amount is almost twice as large on glass compared to TeflonAF for both isomers. The adsorption rate for the trans-isomers on both surfaces is similar, but the desorption rate of the trans-isomers is faster at the glass-water interface than at the Teflon-water interface. This result demonstrates that the trans-isomers have higher affinity for the glass surface, so the trans-to-cis ratios on glass and TeflonAF are 80/1 and 2/1, respectively, with similar trends for all three surfactant types.
The quantitative analysis of microstructural features is a key to understanding the micromechanical behavior of metal matrix composites (MMCs), which is a premise for their use in practice. Herein, a 3D microstructural characterization of a five-phase MMC is performed by synchrotron X-ray computed tomography (SXCT). A workflow for advanced deep learning-based segmentation of all individual phases in SXCT data is shown using a fully convolutional neural network with U-net architecture. High segmentation accuracy is achieved with a small amount of training data. This enables extracting unprecedently precise microstructural parameters (e.g., volume fractions and particle shapes) to be input, e.g., in micromechanical models.
Alone but not lonely
(2020)
Context. Hot subdwarfs are core-helium burning stars that show lower masses and higher temperatures than canonical horizontal branch stars. They are believed to be formed when a red giant suffers an extreme mass-loss episode. Binary interaction is suggested to be the main formation channel, but the high fraction of apparently single hot subdwarfs (up to 30%) has prompted single star formation scenarios to be proposed.Aims. We investigate the possibility that hot subdwarfs could form without interaction by studying wide binary systems. If single formation scenarios were possible, there should be hot subdwarfs in wide binaries that have undergone no interaction.Methods. Angular momentum accretion during interaction is predicted to cause the hot subdwarf companion to spin up to the critical velocity. The effect of this should still be observable given the timescales of the hot subdwarf phase. To study the rotation rates of companions, we have analysed light curves from the Transiting Exoplanet Survey Satellite for all known hot subdwarfs showing composite spectral energy distributions indicating the presence of a main sequence wide binary companion. If formation without interaction were possible, that would also imply the existence of hot subdwarfs in very wide binaries that are not predicted to interact. To identify such systems, we have searched for common proper motion companions with projected orbital distances of up to 0.1 pc to all known spectroscopically confirmed hot subdwarfs using Gaia DR2 astrometry.Results. We find that the companions in composite hot subdwarfs show short rotation periods when compared to field main sequence stars. They display a triangular-shaped distribution with a peak around 2.5 days, similar to what is observed for young open clusters. We also report a shortage of hot subdwarfs with candidate common proper motion companions. We identify only 16 candidates after probing 2938 hot subdwarfs with good astrometry. Out of those, at least six seem to be hierarchical triple systems, in which the hot subdwarf is part of an inner binary.Conclusions. The observed distribution of rotation rates for the companions in known wide hot subdwarf binaries provides evidence of previous interaction causing spin-up. Additionally, there is a shortage of hot subdwarfs in common proper motion pairs, considering the frequency of such systems among progenitors. These results suggest that binary interaction is always required for the formation of hot subdwarfs.
Droughts in tropical South America have an imminent and severe impact on the Amazon rainforest and affect the livelihoods of millions of people. Extremely dry conditions in Amazonia have been previously linked to sea surface temperature (SST) anomalies in the adjacent tropical oceans. Although the sources and impacts of such droughts have been widely studied, establishing reliable multi-year lead statistical forecasts of their occurrence is still an ongoing challenge. Here, we further investigate the relationship between SST and rainfall anomalies using a complex network approach. We identify four ocean regions which exhibit the strongest overall SST correlations with central Amazon rainfall, including two particularly prominent regions in the northern and southern tropical Atlantic. Based on the time-dependent correlation between SST anomalies in these two regions alone, we establish a new early-warning method for droughts in the central Amazon basin and demonstrate its robustness in hindcasting past major drought events with lead-times up to 18 months.
The unidentified very-high-energy (VHE; E > 0.1 TeV) gamma -ray source, HESS J1826-130, was discovered with the High Energy Stereoscopic System (HESS) in the Galactic plane. The analysis of 215 h of HESS data has revealed a steady gamma -ray flux from HESS J1826-130, which appears extended with a half-width of 0.21 degrees +/- 0.02 <br /> (stat)degrees <br /> stat degrees +/- 0.05 <br /> (sys)degrees sys degrees . The source spectrum is best fit with either a power-law function with a spectral index Gamma = 1.78 +/- 0.10(stat) +/- 0.20(sys) and an exponential cut-off at 15.2 <br /> (+5.5)(-3.2) -3.2+5.5 TeV, or a broken power-law with Gamma (1) = 1.96 +/- 0.06(stat) +/- 0.20(sys), Gamma (2) = 3.59 +/- 0.69(stat) +/- 0.20(sys) for energies below and above E-br = 11.2 +/- 2.7 TeV, respectively. The VHE flux from HESS J1826-130 is contaminated by the extended emission of the bright, nearby pulsar wind nebula, HESS J1825-137, particularly at the low end of the energy spectrum. Leptonic scenarios for the origin of HESS J1826-130 VHE emission related to PSR J1826-1256 are confronted by our spectral and morphological analysis. In a hadronic framework, taking into account the properties of dense gas regions surrounding HESS J1826-130, the source spectrum would imply an astrophysical object capable of accelerating the parent particle population up to greater than or similar to 200 TeV. Our results are also discussed in a multiwavelength context, accounting for both the presence of nearby supernova remnants, molecular clouds, and counterparts detected in radio, X-rays, and TeV energies.
Concurrent observation technologies have made high-precision real-time data available in large quantities. Data assimilation (DA) is concerned with how to combine this data with physical models to produce accurate predictions. For spatial-temporal models, the ensemble Kalman filter with proper localisation techniques is considered to be a state-of-the-art DA methodology. This article proposes and investigates a localised ensemble Kalman Bucy filter for nonlinear models with short-range interactions. We derive dimension-independent and component-wise error bounds and show the long time path-wise error only has logarithmic dependence on the time range. The theoretical results are verified through some simple numerical tests.
We study populations of globally coupled noisy rotators (oscillators with inertia) allowing a nonequilibrium transition from a desynchronized state to a synchronous one (with the nonvanishing order parameter). The newly developed analytical approaches resulted in solutions describing the synchronous state with constant order parameter for weakly inertial rotators, including the case of zero inertia, when the model is reduced to the Kuramoto model of coupled noise oscillators. These approaches provide also analytical criteria distinguishing supercritical and subcritical transitions to the desynchronized state and indicate the universality of such transitions in rotator ensembles. All the obtained analytical results are confirmed by the numerical ones, both by direct simulations of the large ensembles and by solution of the associated Fokker-Planck equation. We also propose generalizations of the developed approaches for setups where different rotators parameters (natural frequencies, masses, noise intensities, strengths and phase shifts in coupling) are dispersed.
We study populations of globally coupled noisy rotators (oscillators with inertia) allowing a nonequilibrium transition from a desynchronized state to a synchronous one (with the nonvanishing order parameter). The newly developed analytical approaches resulted in solutions describing the synchronous state with constant order parameter for weakly inertial rotators, including the case of zero inertia, when the model is reduced to the Kuramoto model of coupled noise oscillators. These approaches provide also analytical criteria distinguishing supercritical and subcritical transitions to the desynchronized state and indicate the universality of such transitions in rotator ensembles. All the obtained analytical results are confirmed by the numerical ones, both by direct simulations of the large ensembles and by solution of the associated Fokker-Planck equation. We also propose generalizations of the developed approaches for setups where different rotators parameters (natural frequencies, masses, noise intensities, strengths and phase shifts in coupling) are dispersed.
Organic solar cells are currently experiencing a second golden age thanks to the development of novel non-fullerene acceptors (NFAs). Surprisingly, some of these blends exhibit high efficiencies despite a low energy offset at the heterojunction. Herein, free charge generation in the high-performance blend of the donor polymer PM6 with the NFA Y6 is thoroughly investigated as a function of internal field, temperature and excitation energy. Results show that photocurrent generation is essentially barrierless with near-unity efficiency, regardless of excitation energy. Efficient charge separation is maintained over a wide temperature range, down to 100 K, despite the small driving force for charge generation. Studies on a blend with a low concentration of the NFA, measurements of the energetic disorder, and theoretical modeling suggest that CT state dissociation is assisted by the electrostatic interfacial field which for Y6 is large enough to compensate the Coulomb dissociation barrier.
Bioinspired confinement of upconversion nanoparticles for improved performance in aqueous solution
(2020)
The resonance energy transfer (RET) from NaYF4:Yb,Er upconverting nanoparticles (UNCPs) to a dye (5-carboxytetramethylrhodamine (TAMRA)) was investigated by photoluminescence experiments and microscale thermophoresis (MST). The dye was excited via RET from the UCNPs which was excited in the near-infrared (NIR). The change of the dye diffusion speed (free vs coupled) was investigated by MST. RET shows significant changes in the decay times of the dye as well as of the UCNPs. MST reveals significant changes in the diffusion speed. A unique amphiphilic coating polymer (customized mussel protein (CMP) polymer) for UCNP surface coating was used, which mimics blood protein adsorption and mussel food protein adhesion to transfer the UCNP into the aqueous phase and to allow surface functionalization. The CMP provides very good water dispersibility to the UCNPs and minimizes ligand exchange and subsequent UCNP aging reactions because of the interlinkage of the CMP on the UCNP surface. Moreover, CMP provides N-3-functional groups for dick chemistry-based functionalization demonstrated with the dye 5-carboxytetramethylrhodamine (TAMRA). This establishes the principle coupling scheme for suitable biomarkers such as antibodies. The CMP provides very stable aqueous UCNP dispersions that are storable up to 3 years in a fridge at 5 degrees C without dissolution or coagulation. The outstanding properties of CMP in shielding the UCNP from unwanted solvent effects is reflected in the distinct increase of the photoluminescence decay times after UCNP functionalization. The UCNP-to-TAMRA energy transfer is also spectroscopically investigated at low temperatures (4-200 K), revealing that one of the two green Er(III) emission bands contributes the major part to the energy transfer. The TAMRA fluorescence decay time increases by a factor of 9500 from 2.28 ns up to 22 mu s due to radiationless energy transfer from the UCNP after NIR excitation of the latter. This underlines the unique properties of CMP as a versatile capping ligand for distinctly improving the UCNPs' performance in aqueous solutions, for coupling of biomolecules, and for applications for in vitro and in vivo experiments using UCNPs as optical probes in life science applications.
What is the optimal distribution of two types of crystalline phases on the surface of icosahedral shells, such as of many viral capsids? We here investigate the distribution of a thin layer of soft material on a crystalline convex icosahedral shell. We demonstrate how the shapes of spherical viruses can be understood from the perspective of elasticity theory of thin two-component shells. We develop a theory of shape transformations of an icosahedral shell upon addition of a softer, but still crystalline, material onto its surface. We show how the soft component "invades" the regions with the highest elastic energy and stress imposed by the 12 topological defects on the surface. We explore the phase diagram as a function of the surface fraction of the soft material, the shell size, and the incommensurability of the elastic moduli of the rigid and soft phases. We find that, as expected, progressive filling of the rigid shell by the soft phase starts from the most deformed regions of the icosahedron. With a progressively increasing soft-phase coverage, the spherical segments of domes are filled first (12 vertices of the shell), then the cylindrical segments connecting the domes (30 edges) are invaded, and, ultimately, the 20 flat faces of the icosahedral shell tend to be occupied by the soft material. We present a detailed theoretical investigation of the first two stages of this invasion process and develop a model of morphological changes of the cone structure that permits noncircular cross sections. In conclusion, we discuss the biological relevance of some structures predicted from our calculations, in particular for the shape of viral capsids.
The performance of the recently commissioned spectrometer PEAXIS for resonant inelastic soft X-ray scattering (RIXS) and X-ray photoelectron spectroscopy and its hosting beamline U41-PEAXIS at the BESSY II synchrotron are characterized. The beamline provides linearly polarized light from 180 eV to 1600 eV allowing for RIXS measurements in the range 200-1200 eV. The monochromator optics can be operated in different configurations to provide either high flux with up to 10(12) photons s(-1) within the focal spot at the sample or high energy resolution with a full width at half maximum of <40 meV at an incident photon energy of similar to 400 eV. The measured total energy resolution of the RIXS spectrometer is in very good agreement with theoretically predicted values obtained by ray-tracing simulations. PEAXIS features a 5 m-long RIXS spectrometer arm that can be continuously rotated about the sample position by 106 degrees within the horizontal photon scattering plane, thus enabling the study of momentum-transfer-dependent excitations. Selected scientific examples are presented to demonstrate the instrument capabilities, including measurements of excitations in single-crystalline NiO and in liquid acetone employing a fluid cell sample manipulator. Planned upgrades of the beamline and the RIXS spectrometer to further increase the energy resolution to similar to 100 meV at 1000 eV incident photon energy are discussed.
The contamination of barley by molds on the field or in storage leads to the spoilage of grain and the production of mycotoxins, which causes major economic losses in malting facilities and breweries. Therefore, on-site detection of hidden fungus contaminations in grain storages based on the detection of volatile marker compounds is of high interest. In this work, the volatile metabolites of 10 different fungus species are identified by gas chromatography (GC) combined with two complementary mass spectrometric methods, namely, electron impact (EI) and chemical ionization at atmospheric pressure (APCI)-mass spectrometry (MS). The APCI source utilizes soft X-radiation, which enables the selective protonation of the volatile metabolites largely without side reactions. Nearly 80 volatile or semivolatile compounds from different substance classes, namely, alcohols, aldehydes, ketones, carboxylic acids, esters, substituted aromatic compounds, alkenes, terpenes, oxidized terpenes, sesquiterpenes, and oxidized sesquiterpenes, could be identified. The profiles of volatile and semivolatile metabolites of the different fungus species are characteristic of them and allow their safe differentiation. The application of the same GC parameters and APCI source allows a simple method transfer from MS to ion mobility spectrometry (IMS), which permits on-site analyses of grain stores. Characterization of IMS yields limits of detection very similar to those of APCI-MS. Accordingly, more than 90% of the volatile metabolites found by APCI-MS were also detected in IMS. In addition to different fungus genera, different species of one fungus genus could also be differentiated by GC-IMS.
Bacterial chemotaxis-a fundamental example of directional navigation in the living world-is key to many biological processes, including the spreading of bacterial infections. Many bacterial species were recently reported to exhibit several distinct swimming modes-the flagella may, for example, push the cell body or wrap around it. How do the different run modes shape the chemotaxis strategy of a multimode swimmer? Here, we investigate chemotactic motion of the soil bacterium Pseudomonas putida as a model organism. By simultaneously tracking the position of the cell body and the configuration of its flagella, we demonstrate that individual run modes show different chemotactic responses in nutrition gradients and, thus, constitute distinct behavioral states. On the basis of an active particle model, we demonstrate that switching between multiple run states that differ in their speed and responsiveness provides the basis for robust and efficient chemotaxis in complex natural habitats.
Laser-induced breakdown spectroscopy (LIBS) analysers are becoming increasingly common for material classification purposes. However, to achieve good classification accuracy, mostly noncompact units are used based on their stability and reproducibility. In addition, computational algorithms that require significant hardware resources are commonly applied. For performing measurement campaigns in hard-to-access environments, such as mining sites, there is a need for compact, portable, or even handheld devices capable of reaching high measurement accuracy. The optics and hardware of small (i.e., handheld) devices are limited by space and power consumption and require a compromise of the achievable spectral quality. As long as the size of such a device is a major constraint, the software is the primary field for improvement. In this study, we propose a novel combination of handheld LIBS with non-negative tensor factorisation to investigate its classification capabilities of copper minerals. The proposed approach is based on the extraction of source spectra for each mineral (with the use of tensor methods) and their labelling based on the percentage contribution within the dataset. These latent spectra are then used in a regression model for validation purposes. The application of such an approach leads to an increase in the classification score by approximately 5% compared to that obtained using commonly used classifiers such as support vector machines, linear discriminant analysis, and the k-nearest neighbours algorithm.
A comet is a highly dynamic object, undergoing a permanent state of change. These changes have to be carefully classified and considered according to their intrinsic temporal and spatial scales. The Rosetta mission has, through its contiguous in-situ and remote sensing coverage of comet 67P/Churyumov-Gerasimenko (hereafter 67P) over the time span of August 2014 to September 2016, monitored the emergence, culmination, and winding down of the gas and dust comae. This provided an unprecedented data set and has spurred a large effort to connect in-situ and remote sensing measurements to the surface. In this review, we address our current understanding of cometary activity and the challenges involved when linking comae data to the surface. We give the current state of research by describing what we know about the physical processes involved from the surface to a few tens of kilometres above it with respect to the gas and dust emission from cometary nuclei. Further, we describe how complex multidimensional cometary gas and dust models have developed from the Halley encounter of 1986 to today. This includes the study of inhomogeneous outgassing and determination of the gas and dust production rates. Additionally, the different approaches used and results obtained to link coma data to the surface will be discussed. We discuss forward and inversion models and we describe the limitations of the respective approaches. The current literature suggests that there does not seem to be a single uniform process behind cometary activity. Rather, activity seems to be the consequence of a variety of erosion processes, including the sublimation of both water ice and more volatile material, but possibly also more exotic processes such as fracture and cliff erosion under thermal and mechanical stress, sub-surface heat storage, and a complex interplay of these processes. Seasons and the nucleus shape are key factors for the distribution and temporal evolution of activity and imply that the heliocentric evolution of activity can be highly individual for every comet, and generalisations can be misleading.
We present a diffusion-based simulation and theoretical models for explanation of the photoluminescence (PL) emission intensity in semiconductor nanoplatelets. It is shown that the shape of the PL intensity curves can be reproduced by the interplay of recombination, diffusion and trapping of excitons. The emission intensity at short times is purely exponential and is defined by recombination. At long times, it is governed by the release of excitons from surface traps and is characterized by a power-law tail. We show that the crossover from one limit to another is controlled by diffusion properties. This intermediate region exhibits a rich behaviour depending on the value of diffusivity. The proposed approach reproduces all the features of experimental curves measured for different nanoplatelet systems.
This paper discusses the fitting of linear state space models to given multivariate time series in the presence of constraints imposed on the four main parameter matrices of these models. Constraints arise partly from the assumption that the models have a block-diagonal structure, with each block corresponding to an ARMA process, that allows the reconstruction of independent source components from linear mixtures, and partly from the need to keep models identifiable. The first stage of parameter fitting is performed by the expectation maximisation (EM) algorithm. Due to the identifiability constraint, a subset of the diagonal elements of the dynamical noise covariance matrix needs to be constrained to fixed values (usually unity). For this kind of constraints, so far, no closed-form update rules were available. We present new update rules for this situation, both for updating the dynamical noise covariance matrix directly and for updating a matrix square-root of this matrix. The practical applicability of the proposed algorithm is demonstrated by a low-dimensional simulation example. The behaviour of the EM algorithm, as observed in this example, illustrates the well-known fact that in practical applications, the EM algorithm should be combined with a different algorithm for numerical optimisation, such as a quasi-Newton algorithm.
Quasiuniversal relations between the tidal deformability and the quadrupole moment of neutron stars are predicted by theoretical computations, but have not been measured experimentally. We simulate 120 binary neutron star sources and find that Advanced LIGO and Advanced Virgo at design sensitivity could find possible deviations from predicted relations if the neutron stars are highly spinning. A network of envisaged third generation detectors will even allow extracting such relations, providing new tests of general relativity and nuclear physics predictions.
We consider the emerging dynamics of a separable continuous time random walk (CTRW) in the case when the random walker is biased by a velocity field in a uniformly growing domain. Concrete examples for such domains include growing biological cells or lipid vesicles, biofilms and tissues, but also macroscopic systems such as expanding aquifers during rainy periods, or the expanding Universe. The CTRW in this study can be subdiffusive, normal diffusive or superdiffusive, including the particular case of a Lévy flight. We first consider the case when the velocity field is absent. In the subdiffusive case, we reveal an interesting time dependence of the kurtosis of the particle probability density function. In particular, for a suitable parameter choice, we find that the propagator, which is fat tailed at short times, may cross over to a Gaussian-like propagator. We subsequently incorporate the effect of the velocity field and derive a bi-fractional diffusion-advection equation encoding the time evolution of the particle distribution. We apply this equation to study the mixing kinetics of two diffusing pulses, whose peaks move towards each other under the action of velocity fields acting in opposite directions. This deterministic motion of the peaks, together with the diffusive spreading of each pulse, tends to increase particle mixing, thereby counteracting the peak separation induced by the domain growth. As a result of this competition, different regimes of mixing arise. In the case of Lévy flights, apart from the non-mixing regime, one has two different mixing regimes in the long-time limit, depending on the exact parameter choice: in one of these regimes, mixing is mainly driven by diffusive spreading, while in the other mixing is controlled by the velocity fields acting on each pulse. Possible implications for encounter–controlled reactions in real systems are discussed.
We present an efficient technique for control of synchrony in a globally coupled ensemble by pulsatile action. We assume that we can observe the collective oscillation and can stimulate all elements of the ensemble simultaneously. We pay special attention to the minimization of intervention into the system. The key idea is to stimulate only at the most sensitive phase. To find this phase, we implement an adaptive feedback control. Estimating the instantaneous phase of the collective mode on the fly, we achieve efficient suppression using a few pulses per oscillatory cycle. We discuss the possible relevance of the results for neuroscience, namely, for the development of advanced algorithms for deep brain stimulation, a medical technique used to treat Parkinson's disease.
Corona and the climate
(2020)
We propose Mobius maps as a tool to model synchronization phenomena in coupled phase oscillators. Not only does the map provide fast computation of phase synchronization, it also reflects the underlying group structure of the sinusoidally coupled continuous phase dynamics. We study map versions of various known continuous-time collective dynamics, such as the synchronization transition in the Kuramoto-Sakaguchi model of nonidentical oscillators, chimeras in two coupled populations of identical phase oscillators, and Kuramoto-Battogtokh chimeras on a ring, and demonstrate similarities and differences between the iterated map models and their known continuous-time counterparts.
Employing extensive Monte Carlo computer simulations, we investigate in detail the properties of multichain adsorption of charged flexible polyelectrolytes (PEs) onto oppositely charged spherical nanoparticles (SNPs). We quantify the conditions of critical adsorption-the phase-separation curve between the adsorbed and desorbed states of the PEs-as a function of the SNP surface-charge density and the concentration of added salt. We study the degree of fluctuations of the PE-SNP electrostatic binding energy, which we use to quantify the emergence of the phase subtransitions, including a series of partially adsorbed PE configurations. We demonstrate how the phase-separation adsorption-desorption boundary shifts and splits into multiple subtransitions at low-salt conditions, thereby generalizing and extending the results for critical adsorption of a single PE onto the SNP. The current findings are relevant for finite concentrations of PEs around the attracting SNP, such as the conditions for PE adsorption onto globular proteins carrying opposite electric charges.
The Cattaneo or telegrapher's equation describes the crossover from initial ballistic to normal diffusion. Here we study and survey time-fractional generalisations of this equation that are shown to produce the crossover of the mean squared displacement from superdiffusion to subdiffusion. Conditional solutions are derived in terms of Fox H-functions and the dth-order moments as well as the diffusive flux of the different models are derived. Moreover, the concept of the distribution-like is proposed as an alternative to the probability density function.
The paper is motivated by some inconsistencies and contradictions present in the literature on the calculation of the so-called diffraction elastic constants. In an attempt at unifying the views that the two communities of Materials Science and Mechanics of Materials have on the subject, we revisit and define the terminology used in the field. We also clarify the limitations of the commonly used approaches and show that a unified methodology is also applicable to textured materials with a nearly arbitrary grain shape. We finally compare the predictions based on this methodology with experimental data obtained by in situ synchrotron radiation diffraction on additively manufactured Ti-6Al-4V alloy. We show that (a) the transverse isotropy of the material yields good agreement between the best-fit isotropy approximation (equivalent to the classic Kroner's model) and the experimental data and (b) the use of a general framework allows the calculation of all components of the tensor of diffraction elastic constants, which are not easily measurable by diffraction methods. This allows us to extend the current state-of-the-art with a predictive tool.
Here, piezoelectric transducers consisting of a P(VDF-TrFE) layer with either silver or PEDOT:PSS screen-printed electrodes are studied. The influence of electrodes on the dielectric and electroacoustic properties are studied in dielectric-spectroscopy and ferroelectric-hysteresis measurements. Only when both the bottom and the top electrodes are made of silver, the typical dielectric relaxation of the P(VDF-TrFE) layer is clearly observed. When one or two of the electrodes are of PEDOT:PSS, a Debye-like relaxation is present. Compared with silver electrodes, PEDOT:PSS electrodes allow for moderate self-healing. Consequently, samples with bottom and top PEDOT:PSS electrodes can be poled to saturation, while samples with silver electrodes can hardly be poled to saturation due to destructive electric breakdown. Acoustic transducer measurements show that silver electrodes facilitate higher and broader frequency operation, while PEDOT:PSS electrodes bring slightly lower total harmonic distortion. Overall, the acoustic performance shows no significant deviations between differently electroded samples so that silver electrodes do not offer any advantages for the transducers studied here due to their much higher tendency for destructive electric breakdown.
Diffusion of antibiotics through a biofilm in the presence of diffusion and absorption barriers
(2020)
We propose a model of antibiotic diffusion through a bacterial biofilm when diffusion and/or absorption barriers develop in the biofilm. The idea of this model is: We deduce details of the diffusion process in a medium in which direct experimental study is difficult, based on probing diffusion in external regions. Since a biofilm has a gel-like consistency, we suppose that subdiffusion of particles in the biofilm may occur. To describe this process we use a fractional subdiffusion-absorption equation with an adjustable anomalous diffusion exponent. The boundary conditions at the boundaries of the biofilm are derived by means of a particle random walk model on a discrete lattice leading to an expression involving a fractional time derivative. We show that the temporal evolution of the total amount of substance that has diffused through the biofilm explicitly depends on whether there is antibiotic absorption in the biofilm. This fact is used to experimentally check for antibiotic absorption in the biofilm and if subdiffusion and absorption parameters of the biofilm change over time. We propose a four-stage model of antibiotic diffusion in biofilm based on the following physical characteristics: whether there is absorption of the antibiotic in the biofilm and whether all biofilm parameters remain unchanged over time. The biological interpretation of the stages, in particular their relation with the bacterial defense mechanisms, is discussed. Theoretical results are compared with empirical results of ciprofloxacin diffusion through Pseudomonas aeruginosa biofilm, and ciprofloxacin and gentamicin diffusion through Proteus mirabilis biofilm.
X-ray computed tomography has many applications in materials science and non-destructive testing. While the standard filtered back-projection reconstruction of the radiographic datasets is fast and simple, it typically fails in returning accurate results from missing or inconsistent projections. Among the alternative techniques that have been proposed to handle such data is the Direct Iterative REconstruction of Computed Tomography Trajectories (DIRECTT) algorithm. We describe a new approach to the algorithm, which significantly decreases the computational time while achieving a better reconstruction quality than that of other established algorithms.
We discuss the effect of molecular symmetry on coherent tunneling in symmetric double-well potentials whose two molecular equilibrium configurations are interconverted by nuclear permutations. This is illustrated with vibrational tunneling in ammonia molecules, electronic tunneling in the dihydrogen cation, and laser-induced rotational tunneling of homonuclear diatomics. In this contribution, we reexamine the textbook picture of coherent tunneling in such potentials, which is depicted with a wavepacket shuttling back and forth between the two potential-wells. We show that the common application of this picture to the aforementioned molecules contravenes the principle of the indistinguishability of identical particles. This conflict originates from the sole consideration of the dynamics of the tunneling-mode, connecting the double-well energy minima, and complete omission of all the remaining molecular degrees of freedom. This gives rise to double-well wavepackets that are nonsymmetric under nuclear permutations. To obey quantum statistics, we show that the double-well eigenstates composing these wavepackets must be entangled with the wavefunctions that describe all the omitted molecular modes. These wavefunctions have compensating and opposite nuclear permutation symmetry. This in turn leads to complete quenching of interference effects behind localization in one potential-well or another. Indeed, we demonstrate that the reduced density of probability of the symmetrized molecular wavefunction, where all the molecular coordinates but the tunneling-mode are integrated out, is symmetrically distributed over the two potential-wells, at all times. This applies to any multilevel wavepacket of isotropic or fully aligned symmetric double-well achiral molecules. However, in the case of coherent electronic or vibrational tunneling, fully aligned molecules may exhibit dynamical localization in the space-fixed frame, where the tunneling-mode density shuttles between the opposite directions of the alignment axis. This dynamical spatial-localization results from linear combinations of molecular states that have opposite parity. In summary, this study shows that dynamical localization of the tunneling-mode density on either of the two indistinguishable molecular equilibrium configurations of symmetric double-well achiral molecules is forbidden by quantum statistics, whereas its dynamical localization in the space-fixed frame is allowed by parity. The subtle distinction between these two types of localization has far-reaching implications in the interpretation of many ultrafast molecular dynamics experiments.
We show that, although the equilibrium band dispersion of the Shockley-type surface state of two-dimensional Au(111) quantum films grown on W(110) does not deviate from the expected free-electron-like behavior, its nonequilibrium energy-momentum dispersion probed by time- and angle-resolved photoemission exhibits a remarkable kink above the Fermi level due to a significant enhancement of the effective mass. The kink is pronounced for certain thicknesses of the Au quantum well and vanishes in the very thin limit. We identify the kink as induced by the coupling between the Au(111) surface state and emergent quantum-well states which probe directly the buried gold-tungsten interface. The signatures of the coupling are further revealed by our time-resolved measurements which show that surface state and quantum-well states thermalize together behaving as dynamically locked electron populations. In particular, relaxation of hot carriers following laser excitation is similar for both surface state and quantum-well states and much slower than expected for a bulk metallic system. The influence of quantum confinement on the interplay between elementary scattering processes of the electrons at the surface and ultrafast carrier transport in the direction perpendicular to the surface is shown to be the reason for the slow electron dynamics.
Consequences of fluctuating microscopic conductivity in mean-field electrodynamics of turbulent fluids are formulated and discussed. If the conductivity fluctuations are assumed to be uncorrelated with the velocity fluctuations then only the turbulence-originated magnetic diffusivity of the fluid is reduced and the decay time of a large-scale magnetic field or the cycle times of oscillating turbulent dynamo models are increased. If, however, the fluctuations of conductivity and flow in a certain well-defined direction are correlated, an additional diamagnetic pumping effect results, transporting the magnetic field in the opposite direction to the diffusivity flux vector <eta'u'>. In the presence of global rotation, even for homogeneous turbulence fields, an alpha effect appears. If the characteristic values of the outer core of the Earth or the solar convection zone are applied, the dynamo number of the new alpha effect does not reach supercritical values to operate as an alpha(2)-dynamo but oscillating alpha Omega-dynamos with differential rotation are not excluded.
Electrostatic forces above graphene nanoribbons and edges interpreted as partly hydrogen-free
(2020)
Graphene nanoribbons' electronic transport properties strongly depend on the type of edge, armchair, zigzag or other, and on edge functionalization that can be used for band-gap engineering. For only partly hydrogenated edges interesting magnetic properties are predicted. Electric charge accumulates at edges and corners. Scanning force microscopy has so far shown the centre of graphene nanoribbons with atomic resolution using a quartz crystal tuning fork sensor of high stiffness. Weak long-range electrostatic forces related to the charge accumulation on the edges of graphene nanoribbons could not be imaged so far. Here, we show the electrostatic forces at the corners and edges of graphene nanoribbons are amenable to measurement. We use soft cantilevers and a bimodal imaging technique to combine enhanced sensitivity to weak long-range electrostatic forces with the high resolution of the second-frequency shift. Additionally, in our work the edges of the nanoribbons are mainly hydrogen-free, opening to the route to investigations of partly hydrogenated magnetic nanoribbons.
In classical thermodynamic processes the unavoidable presence of irreversibility, quantified by the entropy production, carries two energetic footprints: the reduction of extractable work from the optimal, reversible case, and the generation of a surplus of heat that is irreversibly dissipated to the environment. Recently it has been shown that in the quantum regime an additional quantum irreversibility occurs that is linked to decoherence into the energy basis. Here we employ quantum trajectories to construct distributions for classical heat and quantum heat exchanges, and show that the heat footprint of quantum irreversibility differs markedly from the classical case. We also quantify how quantum irreversibility reduces the amount of work that can be extracted from a state with coherences. Our results show that decoherence leads to both entropic and energetic footprints which both play an important role in the optimization of controlled quantum operations at low temperature.
In classical thermodynamics irreversibility occurs whenever a non-thermal system is brought into contact with a thermal environment. Using quantum trajectories the authors here establish two energetic footprints of quantum irreversible processes, and find that while quantum irreversibility leads to the occurrence of a quantum heat and a reduction of work production, the two are not linked in the same manner as the classical laws of thermodynamics would dictate.
Thought experiments involving gases and pistons, such as Maxwell's demon and Gibbs' mixing, are central to our understanding of thermodynamics. Here, we present a quantum thermodynamic thought experiment in which the energy transfer from two photonic gases to a piston membrane grows quadratically with the number of photons for indistinguishable gases, while it grows linearly for distinguishable gases. This signature of bosonic bunching may be observed in optomechanical experiments, highlighting the potential of these systems for the realization of thermodynamic thought experiments in the quantum realm.
Estimating global mean sea-level rise and its uncertainties by 2100 and 2300 from an expert survey
(2020)
Sea-level rise projections and knowledge of their uncertainties are vital to make informed mitigation and adaptation decisions. To elicit projections from members of the scientific community regarding future global mean sea-level (GMSL) rise, we repeated a survey originally conducted five years ago. Under Representative Concentration Pathway (RCP) 2.6, 106 experts projected a likely (central 66% probability) GMSL rise of 0.30-0.65 m by 2100, and 0.54-2.15 m by 2300, relative to 1986-2005. Under RCP 8.5, the same experts projected a likely GMSL rise of 0.63-1.32 m by 2100, and 1.67-5.61 m by 2300. Expert projections for 2100 are similar to those from the original survey, although the projection for 2300 has extended tails and is higher than the original survey. Experts give a likelihood of 42% (original survey) and 45% (current survey) that under the high-emissions scenario GMSL rise will exceed the upper bound (0.98 m) of the likely range estimated by the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, which is considered to have an exceedance likelihood of 17%. Responses to open-ended questions suggest that the increases in upper-end estimates and uncertainties arose from recent influential studies about the impact of marine ice cliff instability on the meltwater contribution to GMSL rise from the Antarctic Ice Sheet.
Gadolinium-doped ceria or gadolinium-stabilized ceria (GDC) is an important technical material due to its ability to conduct O2- ions, e.g., used in solid oxide fuel cells operated at intermediate temperature as an electrolyte, diffusion barrier, and electrode component. We have synthesized Ce1-xGdxO2-y:Eu3+ (0 <= x <= 0.4) nanoparticles (11-15 nm) using a scalable spray pyrolysis method, which allows the continuous large-scale technical production of such materials. Introducing Eu3+ ions in small amounts into ceria and GDC as spectroscopic probes can provide detailed information about the atomic structure and local environments and allows us to monitor small structural changes. This study presents a novel approach to structurally elucidate europium-doped Ce1-xGdxO2-y:Eu3+ nanoparticles by way of Eu3+ spectroscopy, processing the spectroscopic data with the multiway decomposition method parallel factor (PARAFAC) analysis. In order to perform the deconvolution of spectra, data sets of excitation wavelength, emission wavelength, and time are required. Room temperature, time-resolved emission spectra recorded at lambda(ex) = 464 nm show that Gd3+ doping results in significantly altered emission spectra compared to pure ceria. The PARAFAC analysis for the pure ceria samples reveals a high-symmetry species (which can also be probed directly via the CeO2 charge transfer band) and a low-symmetry species. The GDC samples yield two low-symmetry spectra in the same experiment. High-resolution emission spectra recorded under cryogenic conditions after probing the D-5(0)-F-7(0) transition at lambda(ex) = 575-583 nm revealed additional variation in the low-symmetry Eu3+ sites in pure ceria and GDC. The total luminescence spectra of CeO2-y:Eu3+ showed Eu3+ ions located in at least three slightly different coordination environments with the same fundamental symmetry, whereas the overall hypsochromic shift and increased broadening of the D-5(0)-F-7(0) excitation in the GDC samples, as well as the broadened spectra after deconvolution point to less homogeneous environments. The data of the Gd3+-containing samples indicates that the average charge density around the Eu3+ ions in the lattice is decreased with increasing Gd3+ and oxygen vacancy concentration. For reference, the Judd-Ofelt parameters of all spectra were calculated. PARAFAC proves to be a powerful tool to analyze lanthanide spectra in crystalline solid materials, which are characterized by numerous Stark transitions and where measurements usually yield a superposition of different contributions to any given spectrum.
We study the extremal properties of a stochastic process xt defined by the Langevin equation ẋₜ =√2Dₜ ξₜ, in which ξt is a Gaussian white noise with zero mean and Dₜ is a stochastic‘diffusivity’, defined as a functional of independent Brownian motion Bₜ.We focus on threechoices for the random diffusivity Dₜ: cut-off Brownian motion, Dₜt ∼ Θ(Bₜ), where Θ(x) is the Heaviside step function; geometric Brownian motion, Dₜ ∼ exp(−Bₜ); and a superdiffusive process based on squared Brownian motion, Dₜ ∼ B²ₜ. For these cases we derive exact expressions for the probability density functions of the maximal positive displacement and of the range of the process xₜ on the time interval ₜ ∈ (0, T).We discuss the asymptotic behaviours of the associated probability density functions, compare these against the behaviour of the corresponding properties of standard Brownian motion with constant diffusivity (Dₜ = D0) and also analyse the typical behaviour of the probability density functions which is observed for a majority of realisations of the stochastic diffusivity process.
Excitable solitons
(2020)
Excitable pulses are among the most widespread dynamical patterns that occur in many different systems, ranging from biological cells to chemical reactions and ecological populations. Traditionally, the mutual annihilation of two colliding pulses is regarded as their prototypical signature. Here we show that colliding excitable pulses may exhibit solitonlike crossover and pulse nucleation if the system obeys a mass conservation constraint. In contrast to previous observations in systems without mass conservation, these alternative collision scenarios are robustly observed over a wide range of parameters. We demonstrate our findings using a model of intracellular actin waves since, on time scales of wave propagations over the cell scale, cells obey conservation of actin monomers. The results provide a key concept to understand the ubiquitous occurrence of actin waves in cells, suggesting why they are so common, and why their dynamics is robust and long-lived.
The PM6:Y6 bulk-heterojunction (BHJ) blend system achieves high short-circuit current (J(SC)) values in thick photovoltaic junctions. Here we analyse these solar cells to understand the observed independence of the short-circuit current upon photoactive layer thickness. We employ a range of optoelectronic measurements and analyses, including Mott-Schottky analysis, CELIV, photoinduced absorption spectroscopy, mobility measurements and simulations, to conclude that, the invariant photocurrent for the devices with different active layer thicknesses is associated with the Y6's diffusion length exceeding 300 nm in case of a 300 nm thick cell. This is despite unintentional doping that occurs in PM6 and the associated space-charge effect, which is expected to be even more profound upon photogeneration. This extraordinarily long diffusion length - which is an order of magnitude larger than typical values for organics - dominates transport in the flat-band region of thick junctions. Our work suggests that the performance of the doped PM6:Y6 organic solar cells resembles that of inorganic devices with diffusion transport playing a pivotal role. Ultimately, this is expected to be a key requirement for the fabrication of efficient, high-photocurrent, thick organic solar cells.
Fluorination of organic spacer impacts on the structural and optical response of 2D perovskites
(2020)
Low-dimensional hybrid perovskites have triggered significant research interest due to their intrinsically tunable optoelectronic properties and technologically relevant material stability. In particular, the role of the organic spacer on the inherent structural and optical features in two-dimensional (2D) perovskites is paramount for material optimization. To obtain a deeper understanding of the relationship between spacers and the corresponding 2D perovskite film properties, we explore the influence of the partial substitution of hydrogen atoms by fluorine in an alkylammonium organic cation, resulting in (Lc)(2)PbI4 and (Lf)(2)PbI4 2D perovskites, respectively. Consequently, optical analysis reveals a clear 0.2 eV blue-shift in the excitonic position at room temperature. This result can be mainly attributed to a band gap opening, with negligible effects on the exciton binding energy. According to Density Functional Theory (DFT) calculations, the band gap increases due to a larger distortion of the structure that decreases the atomic overlap of the wavefunctions and correspondingly bandwidth of the valence and conduction bands. In addition, fluorination impacts the structural rigidity of the 2D perovskite, resulting in a stable structure at room temperature and the absence of phase transitions at a low temperature, in contrast to the widely reported polymorphism in some non-fluorinated materials that exhibit such a phase transition. This indicates that a small perturbation in the material structure can strongly influence the overall structural stability and related phase transition of 2D perovskites, making them more robust to any phase change. This work provides key information on how the fluorine content in organic spacer influence the structural distortion of 2D perovskites and their optical properties which possess remarkable importance for future optoelectronic applications, for instance in the field of light-emitting devices or sensors.
We study the peculiar response of photo-sensitive polymer films irradiated with a certain type of interference pattern where one interfering beam is S-polarized, while the second one is P-polarized. The polymer film, although in a glassy state, deforms following the local polarization distribution of the incident light, and a surface relief grating (SRG) appears whose period is half the optical one. All other types of interference patterns result in the matching of both periods. The topographical response is triggered by the alignment of photo-responsive azobenzene containing polymer side chains orthogonal to the local electrical field, resulting in a bulk birefringence grating (BBG). We investigate the process of dual grating formation (SRG and BBG) in a polymer film utilizing a dedicated set-up that combines probe beam diffraction and atomic force microscopy (AFM) measurements, and permits acquiring in situ and in real-time information about changes in local topography and birefringence. We find that the SRG maxima appear at the positions of linearly polarized light (tilted by 45 degrees relative to the grating vector), causing the formation of the half-period topography. This permits to inscribe symmetric and asymmetric topography gratings with sub-wavelength period, while changing only slightly the polarization of one of the interfering beams. We demonstrate an easy generation of sawtooth profiles (blazed gratings) with adjustable shape. With these results, we have taken a significant step in understanding the photo-induced deformation of azo-polymer films.
The present work offers an explanation on how the long-range interaction of dislocations influences their movement, and therefore the strain, during creep of metals. It is proposed that collective motion of dislocations can be described as a fractional Brownian motion. This explains the noisy appearance of the creep strain signal as a function of time. Such signal is split into a deterministic and a stochastic part. These terms can be related to two kinds of dislocation motions: individual and collective, respectively. The description is consistent with the fractal nature of strain-induced dislocation structures predicated in previous works. Moreover, it encompasses the evolution of the strain rate during all stages of creep, including the tertiary one. Creep data from Al99.8% and Al3.85%Mg tested at different temperatures and stresses are used to validate the proposed ideas: it is found that different creep stages present different diffusion characters, and therefore different dislocation motion character.
Numerous examples for a priori unexpected non-Gaussian behaviour for normal and anomalous diffusion have recently been reported in single-particle tracking experiments. Here, we address the case of non-Gaussian anomalous diffusion in terms of a random-diffusivity mechanism in the presence of power-law correlated fractional Gaussian noise. We study the ergodic properties of this model via examining the ensemble- and time-averaged mean-squared displacements as well as the ergodicity breaking parameter EB quantifying the trajectory-to-trajectory fluctuations of the latter. For long measurement times, interesting crossover behaviour is found as function of the correlation time tau characterising the diffusivity dynamics. We unveil that at short lag times the EB parameter reaches a universal plateau. The corresponding residual value of EB is shown to depend only on tau and the trajectory length. The EB parameter at long lag times, however, follows the same power-law scaling as for fractional Brownian motion. We also determine a corresponding plateau at short lag times for the discrete representation of fractional Brownian motion, absent in the continuous-time formulation. These analytical predictions are in excellent agreement with results of computer simulations of the underlying stochastic processes. Our findings can help distinguishing and categorising certain nonergodic and non-Gaussian features of particle displacements, as observed in recent single-particle tracking experiments.
Nanoporous carbon materials (NCMs) provide the "function" of high specific surface area and thus have large interface area for interactions with surrounding species, which is of particular importance in applications related to adsorption processes. The strength and mechanism of adsorption depend on the pore architecture of the NCMs. In addition, chemical functionalization can be used to induce changes of electron density and/or electron density distribution in the pore walls, thus further modifying the interactions between carbons and guest species. Typical approaches for functionalization of nanoporous materials with regular atomic construction like porous silica, metal-organic frameworks, or zeolites, cannot be applied to NCMs due to their less defined local atomic construction and abundant defects. Therefore, synthetic strategies that offer a higher degree of control over the process of functionalization are needed. Synthetic approaches for covalent functionalization of NCMs, that is, for the incorporation of heteroatoms into the carbon backbone, are critically reviewed with a special focus on strategies following the concept "from molecules to materials." Approaches for coordinative functionalization with metallic species, and the functionalization by nanocomposite formation between pristine carbon materials and heteroatom-containing carbons, are introduced as well. Particular focus is given to the influences of these functionalizations in adsorption-related applications.
We consider the first-passage problem for N identical independent particles that are initially released uniformly in a finite domain Ω and then diffuse toward a reactive area Γ, which can be part of the outer boundary of Ω or a reaction centre in the interior of Ω. For both cases of perfect and partial reactions, we obtain the explicit formulas for the first two moments of the fastest first-passage time (fFPT), i.e., the time when the first out of the N particles reacts with Γ. Moreover, we investigate the full probability density of the fFPT. We discuss a significant role of the initial condition in the scaling of the average fFPT with the particle number N, namely, a much stronger dependence (1/N and 1/N² for partially and perfectly reactive targets, respectively), in contrast to the well known inverse-logarithmic behaviour found when all particles are released from the same fixed point. We combine analytic solutions with scaling arguments and stochastic simulations to rationalise our results, which open new perspectives for studying the relevance of multiple searchers in various situations of molecular reactions, in particular, in living cells.
Classical option pricing schemes assume that the value of a financial asset follows a geometric Brownian motion (GBM). However, a growing body of studies suggest that a simple GBM trajectory is not an adequate representation for asset dynamics, due to irregularities found when comparing its properties with empirical distributions. As a solution, we investigate a generalisation of GBM where the introduction of a memory kernel critically determines the behaviour of the stochastic process. We find the general expressions for the moments, log-moments, and the expectation of the periodic log returns, and then obtain the corresponding probability density functions using the subordination approach. Particularly, we consider subdiffusive GBM (sGBM), tempered sGBM, a mix of GBM and sGBM, and a mix of sGBMs. We utilise the resulting generalised GBM (gGBM) in order to examine the empirical performance of a selected group of kernels in the pricing of European call options. Our results indicate that the performance of a kernel ultimately depends on the maturity of the option and its moneyness.
Glacial-cycle simulations of the Antarctic Ice Sheet with the Parallel Ice Sheet Model (PISM)
(2020)
The Parallel Ice Sheet Model (PISM) is applied to the Antarctic Ice Sheet over the last two glacial cycles (approximate to 210 000 years) with a resolution of 16 km. An ensemble of 256 model runs is analyzed in which four relevant model parameters have been systematically varied using full-factorial parameter sampling. Parameters and plausible parameter ranges have been identified in a companion paper (Albrecht et al., 2020) and are associated with ice dynamics, climatic forcing, basal sliding and bed deformation and represent distinct classes of model uncertainties. The model is scored against both modern and geologic data, including reconstructed grounding-line locations, elevation-age data, ice thickness, surface velocities and uplift rates. An aggregated score is computed for each ensemble member that measures the overall model-data misfit, including measurement uncertainty in terms of a Gaussian error model (Briggs and Tarasov, 2013). The statistical method used to analyze the ensemble simulation results follows closely the simple averaging method described in Pollard et al. (2016).
This analysis reveals clusters of best-fit parameter combinations, and hence a likely range of relevant model and boundary parameters, rather than individual best-fit parameters. The ensemble of reconstructed histories of Antarctic Ice Sheet volumes provides a score-weighted likely range of sea-level contributions since the Last Glacial Maximum (LGM) of 9.4 +/- 4.1m (or 6.5 +/- 2.0 x 10(6) km(3)), which is at the upper range of most previous studies. The last deglaciation occurs in all ensemble simulations after around 12 000 years before present and hence after the meltwater pulse 1A (MWP1a). Our ensemble analysis also provides an estimate of parametric uncertainty bounds for the present-day state that can be used for PISM projections of future sea-level contributions from the Antarctic Ice Sheet.
Several large-scale cryosphere elements such as the Arctic summer sea ice, the mountain glaciers, the Greenland and West Antarctic Ice Sheet have changed substantially during the last century due to anthropogenic global warming. However, the impacts of their possible future disintegration on global mean temperature (GMT) and climate feedbacks have not yet been comprehensively evaluated. Here, we quantify this response using an Earth system model of intermediate complexity. Overall, we find a median additional global warming of 0.43 degrees C (interquartile range: 0.39-0.46 degrees C) at a CO2 concentration of 400 ppm. Most of this response (55%) is caused by albedo changes, but lapse rate together with water vapour (30%) and cloud feedbacks (15%) also contribute significantly. While a decay of the ice sheets would occur on centennial to millennial time scales, the Arctic might become ice-free during summer within the 21st century. Our findings imply an additional increase of the GMT on intermediate to long time scales. The disintegration of cryosphere elements such as the Arctic summer sea ice, mountain glaciers, Greenland and West Antarctica is associated with temperature and radiative feedbacks. In this work, the authors quantify these feedbacks and find an additional global warming of 0.43 degrees C.
We construct an expression for the Green function of a differential operator satisfying nonlocal, homogeneous boundary conditions starting from the fundamental solution of the differential operator. This also provides the solution to the boundary value problem of an inhomogeneous partial differential equation with inhomogeneous, nonlocal boundary conditions. The construction applies for a broad class of linear partial differential equations and linear boundary conditions.
Heterogeneous diffusion processes (HDPs) with space-dependent diffusion coefficients D(x) are found in a number of real-world systems, such as for diffusion of macromolecules or submicron tracers in biological cells. Here, we examine HDPs in quenched-disorder systems with Gaussian colored noise (GCN) characterized by a diffusion coefficient with a power-law dependence on the particle position and with a spatially random scaling exponent. Typically, D(x) is considered to be centerd at the origin and the entire x axis is characterized by a single scaling exponent a. In this work we consider a spatially random scenario: in periodic intervals ("layers") in space D(x) is centerd to the midpoint of each interval. In each interval the scaling exponent alpha is randomly chosen from a Gaussian distribution. The effects of the variation of the scaling exponents, the periodicity of the domains ("layer thickness") of the diffusion coefficient in this stratified system, and the correlation time of the GCN are analyzed numerically in detail. We discuss the regimes of superdiffusion, subdiffusion, and normal diffusion realisable in this system. We observe and quantify the domains where nonergodic and non-Gaussian behaviors emerge in this system. Our results provide new insights into the understanding of weak ergodicity breaking for HDPs driven by colored noise, with potential applications in quenched layered systems, typical model systems for diffusion in biological cells and tissues, as well as for diffusion in geophysical systems.
We study a distribution of times of the first arrivals to absorbing targets in turbulent diffusion, which is due to a multiplicative noise. Two examples of dynamical systems with a multiplicative noise are studied. The first one is a random process according to inhomogeneous diffusion, which is also known as a geometric Brownian motion in the Black-Scholes model. The second model is due to a random processes on a two-dimensional comb, where inhomogeneous advection is possible only along the backbone, while Brownian diffusion takes place inside the branches. It is shown that in both cases turbulent diffusion takes place as the one-dimensional random process with the log-normal distribution in the presence of absorbing targets, which are characterized by the Levy-Smirnov distribution for the first hitting times.
Low donor content solar cells are an intriguing class of photovoltaic device about which there is still considerable discussion with respect to their mode of operation. We have synthesized a series of triphenylamine-based materials for use in low donor content devices with the electron accepting [6,6]-phenyl-C71-butyric acid methyl ester (PC(7)0BM). The triphenylamine-based materials absorb light in the near UV enabling the PC(7)0BM to be be the main light absorbing organic semiconducting material in the solar cell. It was found that the devices did not operate as classical Schottky junctions but rather photocurrent was generated by hole transfer from the photo-excited PC(7)0BM to the triphenylamine-based donors. We found that replacing the methoxy surface groups with methyl groups on the donor material led to a decrease in hole mobility for the neat films, which was due to the methyl substituted materials having the propensity to aggregate. The thermodynamic drive to aggregate was advantageous for the performance of the low donor content (6 wt%) films. It was found that the 6 wt% donor devices generally gave higher performance than devices containing 50 wt% of the donor.
IMDfence
(2020)
Over the past decade, focus on the security and privacy aspects of implantable medical devices (IMDs) has intensified, driven by the multitude of cybersecurity vulnerabilities found in various existing devices. However, due to their strict computational, energy and physical constraints, conventional security protocols are not directly applicable to IMDs. Custom-tailored schemes have been proposed instead which, however, fail to cover the full spectrum of security features that modern IMDs and their ecosystems so critically require. In this paper we propose IMDfence, a security protocol for IMD ecosystems that provides a comprehensive yet practical security portfolio, which includes availability, non-repudiation, access control, entity authentication, remote monitoring and system scalability. The protocol also allows emergency access that results in the graceful degradation of offered services without compromising security and patient safety. The performance of the security protocol as well as its feasibility and impact on modern IMDs are extensively analyzed and evaluated. We find that IMDfence achieves the above security requirements at a mere less than 7% increase in total IMD energy consumption, and less than 14 ms and 9 kB increase in system delay and memory footprint, respectively.
Dielectric elastomer devices operate on the principle of Maxwell stress and their operating performance significantly rely on the elastomer and compliant electrode's electrical and mechanical properties. This paper reports that performing actuation tests at elevated temperatures resulted in an enhanced performance due to the reduction of Young's modulus and the increase of dielectric permittivity. As a result, considerably higher isometric forces and isotonic strains were achieved above the ambient operating temperature. For actuators made of silicone, polyurethane and acrylic elastomers, 166%, 70% and 266% higher isometric forces and 450%, 250% and 54% higher isotonic strains were observed, respectively, when tested at the temperature of 100 degrees C in comparison to ambient temperature values using the same operating voltages. Values of up to 0.4 J kg(-1) and 3.1 W kg(-1) were achieved for the work and power outputs per mass, respectively, on a silicone elastomer driven with a voltage of 1.5 kV at a temperature of 100 degrees C.
Numerical-relativity simulations are essential for studying the last stages of the binary neutron star coalescence. Unfortunately, for stable simulations there is the need to add an artificial low-density atmosphere. Here we discuss a new framework in which we can effectively set the density surrounding the neutron stars to zero to ensure a more accurate simulation. We test our method with a number of single star test cases and for an equal-mass binary neutron star simulation. While the bulk motion of the system is not influenced, and hence there is no improvement with respect to the emitted gravitational-wave signal, we find that the new approach is superior with respect to mass conservation and it allows a much better tracking of outward moving material. This will allow a more accurate simulation of the ejected material and supports the interpretation of present and future multimessenger observations with more accurate numerical-relativity simulations.
We investigate the initiation and early evolution of 12 solar eruptions, including six active-region hot channel and six quiescent filament eruptions, which were well observed by the Solar Dynamics Observatory, as well as by the Solar Terrestrial Relations Observatory for the latter. The sample includes one failed eruption and 11 coronal mass ejections, with velocities ranging from 493 to 2140 km s(-1). A detailed analysis of the eruption kinematics yields the following main results. (1) The early evolution of all events consists of a slow-rise phase followed by a main-acceleration phase, the height-time profiles of which differ markedly and can be best fit, respectively, by a linear and an exponential function. This indicates that different physical processes dominate in these phases, which is at variance with models that involve a single process. (2) The kinematic evolution of the eruptions tends to be synchronized with the flare light curve in both phases. The synchronization is often but not always close. A delayed onset of the impulsive flare phase is found in the majority of the filament eruptions (five out of six). This delay and its trend to be larger for slower eruptions favor ideal MHD instability models. (3) The average decay index at the onset heights of the main acceleration is close to the threshold of the torus instability for both groups of events (although, it is based on a tentative coronal field model for the hot channels), suggesting that this instability initiates and possibly drives the main acceleration.
ISMIP6 Antarctica
(2020)
Ice flow models of the Antarctic ice sheet are commonly used to simulate its future evolution in response to different climate scenarios and assess the mass loss that would contribute to future sea level rise. However, there is currently no consensus on estimates of the future mass balance of the ice sheet, primarily because of differences in the representation of physical processes, forcings employed and initial states of ice sheet models. This study presents results from ice flow model simulations from 13 international groups focusing on the evolution of the Antarctic ice sheet during the period 2015-2100 as part of the Ice Sheet Model Intercomparison for CMIP6 (ISMIP6). They are forced with outputs from a subset of models from the Coupled Model Intercomparison Project Phase 5 (CMIP5), representative of the spread in climate model results. Simulations of the Antarctic ice sheet contribution to sea level rise in response to increased warming during this period varies between 7:8 and 30.0 cm of sea level equivalent (SLE) under Representative Concentration Pathway (RCP) 8.5 scenario forcing. These numbers are relative to a control experiment with constant climate conditions and should therefore be added to the mass loss contribution under climate conditions similar to present-day conditions over the same period. The simulated evolution of the West Antarctic ice sheet varies widely among models, with an overall mass loss, up to 18.0 cm SLE, in response to changes in oceanic conditions. East Antarctica mass change varies between 6 :1 and 8.3 cm SLE in the simulations, with a significant increase in surface mass balance outweighing the increased ice discharge under most RCP 8.5 scenario forcings. The inclusion of ice shelf collapse, here assumed to be caused by large amounts of liquid water ponding at the surface of ice shelves, yields an additional simulated mass loss of 28mm compared to simulations without ice shelf collapse. The largest sources of uncertainty come from the climate forcing, the ocean-induced melt rates, the calibration of these melt rates based on oceanic conditions taken outside of ice shelf cavities and the ice sheet dynamic response to these oceanic changes. Results under RCP 2.6 scenario based on two CMIP5 climate models show an additional mass loss of 0 and 3 cm of SLE on average compared to simulations done under present-day conditions for the two CMIP5 forcings used and display limited mass gain in East Antarctica.
We consider several examples of dynamical systems demonstrating overlapping attractor and repeller. These systems are constructed via introducing controllable dissipation to prototypic models with chaotic dynamics (Anosov cat map, Chirikov standard map, and incompressible three-dimensional flow of the ABC-type on a three-torus) and ergodic non-chaotic behavior (skew-shift map). We employ the Kantorovich-Rubinstein-Wasserstein distance to characterize the difference between the attractor and the repeller, in dependence on the dissipation level.
We report on photoisomerization kinetics of azobenzene containing surfactants in aqueous solution. The surfactant molecule consists of a positively charged trimethylammonium bromide head group, a hydrophobic spacer connecting via 6 to 10 CH2 groups to the azobenzene unit, and the hydrophobic tail of 1 and 3CH(2) groups. Under exposure to light, the azobenzene photoisomerizes from more stable trans- to metastable cis-state, which can be switched back either thermally in dark or by illumination with light of a longer wavelength. The surfactant isomerization is described by a kinetic model of a pseudo first order reaction approaching equilibrium, where the intensity controls the rate of isomerization until the equilibrated state. The rate constants of the trans-cis and cis-trans photoisomerization are calculated as a function of several parameters such as wavelength and intensity of light, the surfactant concentration, and the length of the hydrophobic tail. The thermal relaxation rate from cis- to trans-state is studied as well. The surfactant isomerization shows a different kinetic below and above the critical micellar concentration of the trans isomer due to steric hindrance within the densely packed micelle but does not depend on the spacer length.
Cosmic-Ray neutron sensors are widely used to determine soil moisture on the hectare scale. Precise measurements, especially in the case of mobile application, demand for neutron detectors with high counting rates and high signal-to-noise ratios. For a long time Cosmic Ray Neutron Sensing (CRNS) instruments have relied on He-3 as an efficient neutron converter. Its ongoing scarcity demands for technological solutions using alternative converters, which are Li-6 and B-10. Recent developments lead to a modular neutron detector consisting of several B-10-lined proportional counter tubes, which feature high counting rates via its large surface area. The modularity allows for individual shieldings of different segments within the detector featuring the capability of gaining spectral information about the detected neutrons. This opens the possibility for active signal correction, especially useful when applied to mobile measurements, where the influence of constantly changing near-field to the overall signal should be corrected. Furthermore, the signal-to-noise ratio could be increased by combining pulse height and pulse length spectra to discriminate between neutrons and other environmental radiation. This novel detector therefore combines high-selective counting electronics with large-scale instrumentation technology.
A conducting Taylor-Couette flow with quasi-Keplerian rotation law containing a toroidal magnetic field serves as a mean-field dynamo model of the Tayler-Spruit type. The flows are unstable against non-axisymmetric perturbations which form electromotive forces defining a effect and eddy diffusivity. If both degenerated modes with m = +/- 1 are excited with the same power then the global a effect vanishes and a dynamo cannot work. It is shown, however, that the Tayler instability produces finite alpha effects if only an isolated mode is considered but this intrinsic helicity of the single-mode is too low for an alpha(2) dynamo. Moreover, an alpha Omega dynamo model with quasi-Keplerian rotation requires a minimum magnetic Reynolds number of rotation of Rm similar or equal to 2000 to work. Whether it really works depends on assumptions about the turbulence energy. For a steeper-than-quadratic dependence of the turbulence intensity on the magnetic field, however, dynamos are only excited if the resulting magnetic eddy diffusivity approximates its microscopic value, eta(T) similar or equal to eta. By basically lower or larger eddy diffusivities the dynamo instability is suppressed.
The escape from a potential well is an archetypal problem in the study of stochastic dynamical systems, representing real-world situations from chemical reactions to leaving an established home range in movement ecology. Concurrently, Levy noise is a well-established approach to model systems characterized by statistical outliers and diverging higher order moments, ranging from gene expression control to the movement patterns of animals and humans. Here, we study the problem of Levy noise-driven escape from an almost rectangular, arctangent potential well restricted by two absorbing boundaries, mostly under the action of the Cauchy noise. We unveil analogies of the observed transient dynamics to the general properties of stationary states of Levy processes in single-well potentials. The first-escape dynamics is shown to exhibit exponential tails. We examine the dependence of the escape on the shape parameters, steepness, and height of the arctangent potential. Finally, we explore in detail the behavior of the probability densities of the first-escape time and the last-hitting point.
To analyze stochastic processes, one often uses integral transform (Fourier and Laplace) methods. However, for the time-space coupled cases, e.g. the Levy walk, sometimes the integral transform method may fail. Here we provide a Hermite polynomial expansion approach, being complementary to the integral transform method, to the Levy walk. Two approaches are compared for some already known results. We also consider the generalized Levy walk with parameter dependent velocity. Namely, we consider the Levy walk with velocity which depends on the walking length or on the duration of each step. Some interesting features of the generalized Levy walk are observed, including the special shapes of the probability density function, the first passage time distributions, and various diffusive behaviors of the mean squared displacement.
In this paper, we introduce the phenomenon of light driven diffusioosmotic long-range attraction and repulsion of porous particles under irradiation with UV light. The change in the inter-particle interaction potential is governed by flow patterns generated around single colloids and results in reversible aggregation or separation of the mesoporous silica particles that are trapped at a solid surface. The range of the interaction potential extends to several times the diameter of the particle and can be adjusted by varying the light intensity. The "fuel" of the process is a photosensitive surfactant undergoing photo-isomerization from a more hydrophobic trans-state to a rather hydrophilic cis-state. The surfactant has different adsorption affinities to the particles depending on the isomerization state. The trans-isomer, for example, tends to accumulate in the negatively charged pores of the particles, while the cis-isomer prefers to remain in the solution. This implies that when under UV irradiation cis-isomers are being formed within the pores, they tend to diffuse out readily and generate an excess concentration near the colloid's outer surface, ultimately resulting in the initiation of diffusioosmotic flow. The direction of the flow depends strongly on the dynamic redistribution of the fraction of trans- and cis-isomers near the colloids due to different kinetics of photo-isomerization within the pores as compared to the bulk. The unique feature of the mechanism discussed in the paper is that the long-range mutual repulsion but also the attraction can be tuned by convenient external optical stimuli such as intensity so that a broad variety of experimental situations for manipulation of a particle ensemble can be realized.
Low-dimensional description for ensembles of identical phase oscillators subject to Cauchy noise
(2020)
We study ensembles of globally coupled or forced identical phase oscillators subject to independent white Cauchy noise. We demonstrate that if the oscillators are forced in several harmonics, stationary synchronous regimes can be exactly described with a finite number of complex order parameters. The corresponding distribution of phases is a product of wrapped Cauchy distributions. For sinusoidal forcing, the Ott-Antonsen low-dimensional reduction is recovered.
Levy walks (LWs) are spatiotemporally coupled random-walk processes describing superdiffusive heat conduction in solids, propagation of light in disordered optical materials, motion of molecular motors in living cells, or motion of animals, humans, robots, and viruses. We here investigate a key feature of LWs-their response to an external harmonic potential. In this generic setting for confined motion we demonstrate that LWs equilibrate exponentially and may assume a bimodal stationary distribution. We also show that the stationary distribution has a horizontal slope next to a reflecting boundary placed at the origin, in contrast to correlated superdiffusive processes. Our results generalize LWs to confining forces and settle some longstanding puzzles around LWs.
Machine learning control
(2020)
Recently, the term explainable AI came into discussion as an approach to produce models from artificial intelligence which allow interpretation. For a long time, symbolic regression has been used to produce explainable and mathematically tractable models. In this contribution, we extend previous work on symbolic regression methods to infer the optimal control of a dynamical system given one or several optimization criteria, or cost functions. In earlier publications, network control was achieved by automated machine learning control using genetic programming. Here, we focus on the subsequent path continuation analysis of the mathematical expressions which result from the machine learning model. In particular, we use AUTO to analyze the solution properties of the controlled oscillator system which served as our model. As a result, we show that there is a considerable advantage of explainable symbolic regression models over less accessible neural networks. In particular, the roadmap of future works may be to integrate such analyses into the optimization loop itself to filter out robust solutions by construction.
Inorganic perovskites with cesium (Cs+) as the cation have great potential as photovoltaic materials if their phase purity and stability can be addressed. Herein, a series of inorganic perovskites is studied, and it is found that the power conversion efficiency of solar cells with compositions CsPbI1.8Br1.2, CsPbI2.0Br1.0, and CsPbI2.2Br0.8 exhibits a high dependence on the initial annealing step that is found to significantly affect the crystallization and texture behavior of the final perovskite film. At its optimized annealing temperature, CsPbI1.8Br1.2 exhibits a pure orthorhombic phase and only one crystal orientation of the (110) plane. Consequently, this allows for the best efficiency of up to 14.6% and the longest operational lifetime, T-S80, of approximate to 300 h, averaged of over six solar cells, during the maximum power point tracking measurement under continuous light illumination and nitrogen atmosphere. This work provides essential progress on the enhancement of photovoltaic performance and stability of CsPbI3 - xBrx perovskite solar cells.
The radiation belts of the Earth, filled with energetic electrons, comprise complex and dynamic systems that pose a significant threat to satellite operation. While various models of electron flux both for low and relativistic energies have been developed, the behavior of medium energy (120-600 keV) electrons, especially in the MEO region, remains poorly quantified. At these energies, electrons are driven by both convective and diffusive transport, and their prediction usually requires sophisticated 4D modeling codes. In this paper, we present an alternative approach using the Light Gradient Boosting (LightGBM) machine learning algorithm. The Medium Energy electRon fLux In Earth's outer radiatioN belt (MERLIN) model takes as input the satellite position, a combination of geomagnetic indices and solar wind parameters including the time history of velocity, and does not use persistence. MERLIN is trained on >15 years of the GPS electron flux data and tested on more than 1.5 years of measurements. Tenfold cross validation yields that the model predicts the MEO radiation environment well, both in terms of dynamics and amplitudes o f flux. Evaluation on the test set shows high correlation between the predicted and observed electron flux (0.8) and low values of absolute error. The MERLIN model can have wide space weather applications, providing information for the scientific community in the form of radiation belts reconstructions, as well as industry for satellite mission design, nowcast of the MEO environment, and surface charging analysis.
Context. The High Energy Stereoscopic System Galactic plane survey (HGPS) is to date the most comprehensive census of Galactic gamma -ray sources at very high energies (VHE; 100 GeV <= E <= 100 TeV). As a consequence of the limited sensitivity of this survey, the 78 detected gamma -ray sources comprise only a small and biased subsample of the overall population. The larger part consists of currently unresolved sources, which contribute to large-scale diffuse emission to a still uncertain amount.Aims. We study the VHE gamma -ray source population in the Milky Way. For this purpose population-synthesis models are derived based on the distributions of source positions, extents, and luminosities.Methods. Several azimuth-symmetric and spiral-arm models are compared for spatial source distribution. The luminosity and radius function of the population are derived from the source properties of the HGPS data set and are corrected for the sensitivity bias of the HGPS. Based on these models, VHE source populations are simulated and the subsets of sources detectable according to the HGPS are compared with HGPS sources.Results. The power-law indices of luminosity and radius functions are determined to range between -1.6 and -1.9 for luminosity and -1.1 and -1.6 for radius. A two-arm spiral structure with central bar is discarded as spatial distribution of VHE sources, while azimuth-symmetric distributions and a distribution following a four-arm spiral structure without bar describe the HGPS data reasonably well. The total number of Galactic VHE sources is predicted to be in the range from 800 to 7000 with a total luminosity and flux of (1.6-6.3) x 10(36) ph s(-1) and (3-15) x 10(-10) ph cm(-2) s(-1), respectively.Conclusions. Depending on the model, the HGPS sample accounts for (68-87)% of the emission of the population in the scanned region. This suggests that unresolved sources represent a critical component of the diffuse emission measurable in the HGPS. With the foreseen jump in sensitivity of the Cherenkov Telescope Array, the number of detectable sources is predicted to increase by a factor between 5 and 9.
In this paper, we study the problem of formal verification for Answer Set Programming (ASP), namely, obtaining aformal proofshowing that the answer sets of a given (non-ground) logic programPcorrectly correspond to the solutions to the problem encoded byP, regardless of the problem instance. To this aim, we use a formal specification language based on ASP modules, so that each module can be proved to capture some informal aspect of the problem in an isolated way. This specification language relies on a novel definition of (possibly nested, first order)program modulesthat may incorporate local hidden atoms at different levels. Then,verifyingthe logic programPamounts to prove some kind of equivalence betweenPand its modular specification.
A synthesis route to controlled and dynamic single polymer chain folding is reported. Sequence-controlled macromolecules containing precisely located selenol moieties within a polymer chain are synthesized. Oxidation of selenol functionalities lead to diselenide bridges and induces controlled intramolecular crosslinking to generate single chain collapse. The cyclization process is successfully characterized by SEC as well as by H-1 NMR and 2D HSQC NMR spectroscopies. In order to gain insight on the molecular level to reveal the degree of structural control, the folded polymers are transformed into folded molecular brushes that are known to be visualizable as single molecule structures by AFM. The "grafting onto" approach is performed by using triazolinedione-diene reaction to graft the side chain polymers. A series of folded molecular brushes as well as the corresponding linear controls are synthesized. AFM visualization is proving the cyclization of the folded backbone by showing globular objects, where non-folded brushes show typical worm-like structures. (C) 2019 The Authors. Journal of Polymer Science published by Wiley Periodicals, Inc.
We consider large networks of theta neurons on a ring, synaptically coupled with an asymmetric kernel. Such networks support stable "bumps" of activity, which move along the ring if the coupling kernel is asymmetric. We investigate the effects of the kernel asymmetry on the existence, stability, and speed of these moving bumps using continuum equations formally describing infinite networks. Depending on the level of heterogeneity within the network, we find complex sequences of bifurcations as the amount of asymmetry is varied, in strong contrast to the behavior of a classical neural field model.
Nonstationary coherence-incoherence patterns in nonlocally coupled heterogeneous phase oscillators
(2020)
We consider a large ring of nonlocally coupled phase oscillators and show that apart from stationary chimera states, this system also supports nonstationary coherence-incoherence patterns (CIPs). For identical oscillators, these CIPs behave as breathing chimera states and are found in a relatively small parameter region only. It turns out that the stability region of these states enlarges dramatically if a certain amount of spatially uniform heterogeneity (e.g., Lorentzian distribution of natural frequencies) is introduced in the system. In this case, nonstationary CIPs can be studied as stable quasiperiodic solutions of a corresponding mean-field equation, formally describing the infinite system limit. Carrying out direct numerical simulations of the mean-field equation, we find different types of nonstationary CIPs with pulsing and/or alternating chimera-like behavior. Moreover, we reveal a complex bifurcation scenario underlying the transformation of these CIPs into each other. These theoretical predictions are confirmed by numerical simulations of the original coupled oscillator system.
The determination of the voltage-dependent density of free charge carriers via capacitance spectroscopy is considered an important step in the analysis of emerging photovoltaic technologies, such as organic and perovskite solar cells. In particular, an intimate knowledge of the density of free charge carriers is required for the determination of crucial parameters such as the effective mobility, charge carrier lifetime, nongeminate recombination coefficients, average extraction times, and competition factors. Hence, it is paramount to verify the validity of the commonly employed approaches to obtain the density of free charge carriers. The advantages, drawbacks, and limitations of the most common approaches are investigated in detail and strategies to mitigate misleading values are explored. To this end, two types of nonfullerene organic solar cells based on a PTB7-Th:ITIC-2F blend and a PM6:Y6 blend, respectively, are used as a case study to assess how subsequent analyses of the nongeminate recombination dynamics depend on the chosen approach to calculate the density of free charge carriers via capacitance spectroscopy.
Recently, Nocera and co-workers (J. Am. Chem. Soc. 2018, 140, 13711) demonstrated that triaryl borate Lewis acids facilitate the direct electrochemical reduction of triphenylphosphine oxide (TPPO) to triphenylphosphine (TPP). In the present contribution, we report a quantum chemical study unravelling details of the reaction, which also supports the proposed ECrECi mechanism. Alternative electrochemical routes to TPPO reduction facilitated by other Lewis acids (CH3+), or by photocatalysis at semiconductor surfaces, are also briefly discussed.
The relationship between residual stresses and microstructure associated with a laser powder bed fusion (LPBF) IN718 alloy has been investigated on specimens produced with three different scanning strategies (unidirectional Y-scan, 90 degrees XY-scan, and 67 degrees Rot-scan). Synchrotron X-ray energy-dispersive diffraction (EDXRD) combined with optical profilometry was used to study residual stress (RS) distribution and distortion upon removal of the specimens from the baseplate. The microstructural characterization of both the bulk and the near-surface regions was conducted using scanning electron microscopy (SEM) and electron backscatter diffraction (EBSD). On the top surfaces of the specimens, the highest RS values are observed in the Y-scan specimen and the lowest in the Rot-scan specimen, while the tendency is inversed on the side lateral surfaces. A considerable amount of RS remains in the specimens after their removal from the baseplate, especially in the Y- and Z-direction (short specimen dimension and building direction (BD), respectively). The distortion measured on the top surface following baseplate thinning and subsequent removal is mainly attributed to the amount of RS released in the build direction. Importantly, it is observed that the additive manufacturing microstructures challenge the use of classic theoretical models for the calculation of diffraction elastic constants (DEC) required for diffraction-based RS analysis. It is found that when the Reuss model is used for the calculation of RS for different crystal planes, as opposed to the conventionally used Kroner model, the results exhibit lower scatter. This is discussed in context of experimental measurements of DEC available in the literature for conventional and additively manufactured Ni-base alloys.
Perovskite semiconductors as the active materials in efficient solar cells exhibit free carrier diffusion lengths on the order of microns at low illumination fluxes and many hundreds of nanometers under 1 sun conditions. These lengthscales are significantly larger than typical junction thicknesses, and thus the carrier transport and charge collection should be expected to be diffusion controlled. A consensus along these lines is emerging in the field. However, the question as to whether the built-in potential plays any role is still of matter of some conjecture. This important question using phase-sensitive photocurrent measurements and theoretical device simulations based upon the drift-diffusion framework is addressed. In particular, the role of the built-in electric field and charge-selective transport layers in state-of-the-art p-i-n perovskite solar cells comparing experimental findings and simulation predictions is probed. It is found that while charge collection in the junction does not require a drift field per se, a built-in potential is still needed to avoid the formation of reverse electric fields inside the active layer, and to ensure efficient extraction through the charge transport layers.
Understanding the recombination dynamics of organic and perovskite solar cells has been a crucial prerequisite in the steadily increasing performance of these promising new types of photovoltaics. Surface recombination in particular has turned out to be one of the last remaining roadblocks, which specifically reduces the open circuit voltage. In this study, the relationship between the rate of surface recombination and the density of charge carriers is analyzed, revealing a cubic dependence between these two parameters. This hypothesis is then tested and verified with the recombination dynamics of an organic solar cell known to exhibit significant surface recombination and a high energy proton irradiated CH3NH3PbI3 pemvskite solar cell during white light illumination. Incidentally, these results can also explain recombination orders exceeding the commonly known threshold for bimolecular recombination that have been observed in some studies without the need for a charge carrier dependent bimolecular recombination coefficient.
According to established understanding, deep-water formation in the North Atlantic and Southern Ocean keeps the deep ocean cold, counter-acting the downward mixing of heat from the warmer surface waters in the bulk of the world ocean. Therefore, periods of strong Atlantic meridional overturning circulation (AMOC) are expected to coincide with cooling of the deep ocean and warming of the surface waters. It has recently been proposed that this relation may have reversed due to global warming, and that during the past decades a strong AMOC coincides with warming of the deep ocean and relative cooling of the surface, by transporting increasingly warmer waters downward. Here we present multiple lines of evidence, including a statistical evaluation of the observed global mean temperature, ocean heat content, and different AMOC proxies, that lead to the opposite conclusion: even during the current ongoing global temperature rise a strong AMOC warms the surface. The observed weakening of the AMOC has therefore delayed global surface warming rather than enhancing it.
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The overturning circulation in the Atlantic Ocean has weakened in response to global warming, as predicted by climate models. Since it plays an important role in transporting heat, nutrients and carbon, a slowdown will affect global climate processes and the global mean temperature. Scientists have questioned whether this slowdown has worked to cool or warm global surface temperatures. This study analyses the overturning strength and global mean temperature evolution of the past decades and shows that a slowdown acts to reduce the global mean temperature. This is because a slower overturning means less water sinks into the deep ocean in the subpolar North Atlantic. As the surface waters are cold there, the sinking normally cools the deep ocean and thereby indirectly warms the surface, thus less sinking implies less surface warming and has a cooling effect. For the foreseeable future, this means that the slowing of the overturning will likely continue to slightly reduce the effect of the general warming due to increasing greenhouse gas concentrations.
Whereas stable homogenous states of aqueous hydrocarbon solutions are typically observed at high temperatures and pressures far beyond the critical values corresponding to individual components, the stability of such system may be preserved upon transition into the region of metastable states at low temperatures and low pressures. This work is dedicated to the study of the thermal stability of a water-methane mixture formed by cryogenic vapor phase deposition. The obtained thin films were studied using vibrational spectroscopy in the temperature range of 16-180 K. During thermal annealing of the samples, characteristic vibrational C-H modes of methane were monitored alongside the chamber pressure to register both structural changes and desorption of the film material. The obtained results reveal that upon the co-deposition of methane and water, methane molecules appear both in non-bound and trapped states. The observed broadening of the characteristic C-H stretching mode at 3010 cm(-1) upon an increase in temperature of the sample from 16 to 90 K, followed by narrowing of the peak as the temperature is reduced back to 16 K, indicates localization of methane molecules within the water matrix at lower temperatures.
Organic solar cells with large insensitivity to donor polymer molar mass across all acceptor classes
(2020)
Donor polymer number-average molar mass (M-n) has long been known to influence organic photovoltaic (OPV) performance via changes in both the polymer properties and the resulting bulk heterojunction morphology. The exact nature of these M-n effects varies from system to system, although there is generally some intermediate M-n that results in optimal performance. Interestingly, our earlier work with the difluorobenzotriazole (FTAZ)-based donor polymer, paired with either N2200 (polymer acceptor) or PC61BM (fullerene acceptor), PcBm demonstrated <10% variation in power conversion efficiency and a consistent morphology over a large span of M-n (30 kg/mol to over 100 kg/mol). Would such insensitivity to polymer M-n still hold true when prevailing small molecular acceptors were used with FTAZ? To answer this question, we explored the impact of FTAZ on OPVs with ITIC, a high-performance small-molecule fused-ring electron acceptor (FREA). By probing the photovoltaic characteristics of the resulting OPVs, we show that a similar FTAZ mn insensitivity is also found in the FTAZ:ITIC system. This study highlights a single-donor polymer which, when paired with an archetypal fullerene, polymer, and FREA, results in systems that are largely insensitive to donor M. Our results may have implications in polymer batch-to-batch reproducibility, in particular, relaxing the need for tight M-n control during synthesis.
This work demonstrates the production of high-performing p- type and n-type hybrid AgxTe/poly(3,4-ethylenedioxythiopene):polystyrene sulfonic acid (PE-DOT:PSS) thermoelectric materials from the same Te/PEDOT:PSS parent structure during aqueous-based synthesis. All samples were solution-processed and analyzed in thin- film architectures. We were able to demonstrate a power factor of 44 mu W m(-1) K-2 for our highest-performing n-type material. In addition, we were also able to realize a 68% improvement in the power factor of our p-type compositions relative to the parent structure through manipulation of the inorganic nanostructure composition. We demonstrate control over the thermoelectric properties by varying the stoichiometry of AgxTe nanoparticles in AgxTe/PEDOT:PSS hybrid materials via a topotactic chemical transformation process at room temperature. This process offers a simple, low-temperature, and cost-effective route toward the production of both efficient n-type and p-type hybrid thermoelectric materials.
The Paris Climate Agreement aims to keep temperature rise well below 2 degrees C. This implies mitigation costs as well as avoided climate damages. Here we show that independent of the normative assumptions of inequality aversion and time preferences, the agreement constitutes the economically optimal policy pathway for the century. To this end we consistently incorporate a damage-cost curve reproducing the observed relation between temperature and economic growth into the integrated assessment model DICE. We thus provide an intertemporally optimizing cost-benefit analysis of this century's climate problem. We account for uncertainties regarding the damage curve, climate sensitivity, socioeconomic future, and mitigation costs. The resulting optimal temperature is robust as can be understood from the generic temperature-dependence of the mitigation costs and the level of damages inferred from the observed temperature-growth relationship. Our results show that the politically motivated Paris Climate Agreement also represents the economically favourable pathway, if carried out properly.
This work focuses on the dynamics of particles in a confined geometry with position-dependent diffusivity, where the confinement is modelled by a periodic channel consisting of unit cells connected by narrow passage ways. We consider three functional forms for the diffusivity, corresponding to the scenarios of a constant (D ₀), as well as a low (D ₘ) and a high (D d) mobility diffusion in cell centre of the longitudinally symmetric cells. Due to the interaction among the diffusivity, channel shape and external force, the system exhibits complex and interesting phenomena. By calculating the probability density function, mean velocity and mean first exit time with the Itô calculus form, we find that in the absence of external forces the diffusivity D d will redistribute particles near the channel wall, while the diffusivity D ₘ will trap them near the cell centre. The superposition of external forces will break their static distributions. Besides, our results demonstrate that for the diffusivity D d, a high dependence on the x coordinate (parallel with the central channel line) will improve the mean velocity of the particles. In contrast, for the diffusivity D ₘ, a weak dependence on the x coordinate will dramatically accelerate the moving speed. In addition, it shows that a large external force can weaken the influences of different diffusivities; inversely, for a small external force, the types of diffusivity affect significantly the particle dynamics. In practice, one can apply these results to achieve a prominent enhancement of the particle transport in two- or three-dimensional channels by modulating the local tracer diffusivity via an engineered gel of varying porosity or by adding a cold tube to cool down the diffusivity along the central line, which may be a relevant effect in engineering applications. Effects of different stochastic calculi in the evaluation of the underlying multiplicative stochastic equation for different physical scenarios are discussed.
Pre-service physics teachers often do not recognise the relevance for their future career in their university content knowledge courses. A lower perceived relevance can, however, have a negative effect on their motivation and on their academic success. Several intervention studies have been undertaken with the goal to increase this perceived relevance. A previous study shows that conceptual physics problems used in university physics courses are perceived by pre-service physics teachers as more relevant for their future career than regular, quantitative problems. It is however not clear, what the students' meaning of the construct 'relevance' is: what makes a problem more relevant to them than another problem? To answer this question, N = 7 pre-service teachers were interviewed using the repertory grid technique, based on the personal construct theory. Nine physics problems were discussed with regards to their perceived relevance and with regards to problem properties that distinguish these problems from each other. We are able to identify six problem properties that have a positive influence on the perceived relevance. Physics problems that are based on these properties should therefore potentially have a higher perceived relevance, which can have a positive effect on the motivation of the pre-service teachers who solve these problems.
9,10-substituted anthracenes are known for their useful optical properties like fluorescence, which makes them frequently used probes in sensing applications. In this article, we investigate the fundamental photophysical properties of three pyridyl-substituted variants. The nitrogen atoms in the pyridinium six-membered rings are located in the ortho-, meta-, and para-positions in relation to the anthracene core. Absorption, fluorescence, and transient absorption measurements were carried out and were complemented by theoretical calculations. We monitored the photophysics of the anthracene derivatives in chloroform and water investigating the protonated as well as their nonprotonated forms. We found that the optical properties of the nonprotonated forms are strongly determined by the anthracene chromophore, with only small differences to other 9,10-substituted anthracenes, for example diphenyl anthracene. In contrast, protonation leads to a strong decrease in fluorescence intensity and lifetime. Transient absorption measurements and theoretical calculations revealed the formation of a charge-transfer state in the protonated chromophores, where electron density is shifted from the anthracene moiety toward the protonated pyridyl substituents. While the para- and ortho-derivatives' charge transfer is still moderately fluorescent, the meta-derivative is affected much stronger and shows nearly no fluorescence. This nitrogen-atom-position-dependent sensitivity to hydronium activity makes a combination of these fluorophores very attractive for pH-sensing applications covering a broadened pH range.
Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell materials in particular. It can give direct information on the recombination kinetics and processes as well as the internal electrochemical potential of free charge carriers in single semiconductor layers, layer stacks with transport layers, and complete solar cells. The correct evaluation and interpretation of photoluminescence requires the consideration of proper excitation conditions, calibration and application of the appropriate approximations to the rather complex theory, which includes radiative recombination, non-radiative recombination, interface recombination, charge transfer, and photon recycling. In this article, an overview is given of the theory and application to specific halide perovskite compositions, illustrating the variables that should be considered when applying photoluminescence analysis in these materials.
Polarization controlled fine structure of diffraction spots from an optically induced grating
(2020)
We report on the remote control of the fine structure of a diffraction spot from optically induced dual gratings within a photosensitive polymer film. The material contains azobenzene in the polymer side chains and develops a surface relief under two-beam holographic irradiation. The diffraction of a polarized probe beam is sensitive to the orientation of the azobenzene groups forming a permanently stored birefringence grating within the film. We demonstrate that the fine structure of the probe diffraction spot switches from a Gaussian to a hollow or a hollow to a "Saturn"-like structure by a change in polarization. This makes it potentially useful in photonic devices because the beam shape can be easily inverted by an external stimulus.