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- ultraviolet: galaxies (3)
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- 4 (2)
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Institute
- Institut für Physik und Astronomie (4348) (remove)
Non-Markovian diffusion of excitons in layered perovskites and transition metal dichalcogenides
(2022)
The diffusion of excitons in perovskites and transition metal dichalcogenides shows clear anomalous, subdiffusive behaviour in experiments.
In this paper we develop a non-Markovian mobile-immobile model which provides an explanation of this behaviour through paired theoretical and simulation approaches.
The simulation model is based on a random walk on a 2D lattice with randomly distributed deep traps such that the trapping time distribution involves slowly decaying power-law asymptotics.
The theoretical model uses coupled diffusion and rate equations for free and trapped excitons, respectively, with an integral term responsible for trapping.
The model provides a good fitting of the experimental data, thus, showing a way for quantifying the exciton diffusion dynamics.
Inorganic perovskite solar cells show excellent thermal stability, but the reported power conversion efficiencies are still lower than for organic-inorganic perovskites. This is mainly caused by lower open-circuit voltages (V(OC)s). Herein, the reasons for the low V-OC in inorganic CsPbI2Br perovskite solar cells are investigated. Intensity-dependent photoluminescence measurements for different layer stacks reveal that n-i-p and p-i-n CsPbI2Br solar cells exhibit a strong mismatch between quasi-Fermi level splitting (QFLS) and V-OC. Specifically, the CsPbI2Br p-i-n perovskite solar cell has a QFLS-e center dot V-OC mismatch of 179 meV, compared with 11 meV for a reference cell with an organic-inorganic perovskite of similar bandgap. On the other hand, this study shows that the CsPbI2Br films with a bandgap of 1.9 eV have a very low defect density, resulting in an efficiency potential of 20.3% with a MeO-2PACz hole-transporting layer and 20.8% on compact TiO2. Using ultraviolet photoelectron spectroscopy measurements, energy level misalignment is identified as a possible reason for the QFLS-e center dot V-OC mismatch and strategies for overcoming this V-OC limitation are discussed. This work highlights the need to control the interfacial energetics in inorganic perovskite solar cells, but also gives promise for high efficiencies once this issue is resolved.
We consider an array of nearest-neighbor coupled nonlinear autonomous oscillators with quenched ran-dom frequencies and purely conservative coupling. We show that global phase-locked states emerge in finite lattices and study numerically their destruction. Upon change of model parameters, such states are found to become unstable with the generation of localized periodic and chaotic oscillations. For weak nonlinear frequency dispersion, metastability occur akin to the case of almost-conservative systems. We also compare the results with the phase-approximation in which the amplitude dynamics is adiabatically eliminated.
Thermal electrons have gyroradii many orders of magnitude smaller than the finite width of a shock, thus need to be pre-accelerated before they can cross it and be accelerated by diffusive shock acceleration. One region where pre-acceleration may occur is the inner foreshock, which upstream electrons must pass through before any potential downstream crossing. In this paper, we perform a large-scale particle-in-cell simulation that generates a single shock with parameters motivated from supernova remnants. Within the foreshock, reflected electrons excite the oblique whistler instability and produce electromagnetic whistler waves, which comove with the upstream flow and as nonlinear structures eventually reach radii of up to 5 ion-gyroradii. We show that the inner electromagnetic configuration of the whistlers evolves into complex nonlinear structures bound by a strong magnetic field around four times the upstream value. Although these nonlinear structures do not in general interact with cospatial upstream electrons, they resonate with electrons that have been reflected at the shock. We show that they can scatter, or even trap, reflected electrons, confining around 0.8% of the total upstream electron population to the region close to the shock where they can undergo substantial pre-acceleration. This acceleration process is similar to, yet approximately three times more efficient than, stochastic shock drift acceleration.
Traditional inorganic semiconductors can be electronically doped with high precision. Conversely, there is still conjecture regarding the assessment of the electronic doping density in metal-halide perovskites, not to mention of a control thereof. This paper presents a multifaceted approach to determine the electronic doping density for a range of different lead-halide perovskite systems. Optical and electrical characterization techniques, comprising intensity-dependent and transient photoluminescence, AC Hall effect, transfer-length-methods, and charge extraction measurements were instrumental in quantifying an upper limit for the doping density. The obtained values are subsequently compared to the electrode charge per cell volume under short-circuit conditions ( CUbi/eV), which amounts to roughly 10(16) cm(-3). This figure of merit represents the critical limit below which doping-induced charges do not influence the device performance. The experimental results consistently demonstrate that the doping density is below this critical threshold 10(12) cm(-3), which means << CUbi / e V) for all common lead-based metal-halide perovskites. Nevertheless, although the density of doping-induced charges is too low to redistribute the built-in voltage in the perovskite active layer, mobile ions are present in sufficient quantities to create space-charge-regions in the active layer, reminiscent of doped pn-junctions. These results are well supported by drift-diffusion simulations, which confirm that the device performance is not affected by such low doping densities.
With an increasing number of expected gravitational-wave detections of binary neutron star mergers, it is essential that gravitational-wave models employed for the analysis of observational data are able to describe generic compact binary systems. This includes systems in which the individual neutron stars are millisecond pulsars for which spin effects become essential. In this work, we perform numerical-relativity simulations of binary neutron stars with aligned and antialigned spins within a range of dimensionless spins of chi similar to [-0.28, 0.58]. The simulations are performed with multiple resolutions, show a clear convergence order and, consequently, can be used to test existing waveform approximants. We find that for very high spins gravitational-wave models that have been employed for the interpretation of GW170817 and GW190425 arc not capable of describing our numerical-relativity dataset. We verify through a full parameter estimation study in which clear biases in the estimate of the tidal deformability and effective spin are present. We hope that in preparation of the next gravitational-wave observing run of the Advanced LIGO and Advanced Virgo detectors our new set of numerical-relativity data can be used to support future developments of new gravitational-wave models.
Assessing the impact of hydrogen absorption on the characteristics of the Galactic center excess
(2022)
We present a new reconstruction of the distribution of atomic hydrogen in the inner Galaxy that is based on explicit radiation transport modeling of line and continuum emission and a gas-flow model in the barred Galaxy that provides distance resolution for lines of sight toward the Galactic center.
The main benefits of the new gas model are (a) the ability to reproduce the negative line signals seen with the HI4PI survey and (b) the accounting for gas that primarily manifests itself through absorption.
We apply the new model of Galactic atomic hydrogen to an analysis of the diffuse gamma-ray emission from the inner Galaxy, for which an excess at a few GeV was reported that may be related to dark matter.
We find with high significance an improved fit to the diffuse gamma-ray emission observed with the Fermi-LAT, if our new H i model is used to estimate the cosmic-ray induced diffuse gamma-ray emission.
The fit still requires a nuclear bulge at high significance. Once this is included there is no evidence of a dark-matter signal, be it cuspy or cored. But an additional so-called boxy bulge is still favored by the data.
This finding is robust under the variation of various parameters, for example, the excitation temperature of atomic hydrogen, and a number of tests for systematic issues.
Background
Due to physical coupling between mechanical stress and magnetization in ferromagnetic materials, it is assumed in the literature that the distribution of the magnetic stray field corresponds to the internal (residual) stress of the specimen.
The correlation is, however, not trivial, since the magnetic stray field is also influenced by the microstructure and the geometry of component.
The understanding of the correlation between residual stress and magnetic stray field could help to evaluate the integrity of welded components.
Objective
This study aims at understanding the possible correlation of subsurface and bulk residual stress with magnetic stray field in a low carbon steel weld.
Methods
The residual stress was determined by synchrotron X-ray diffraction (SXRD, subsurface region) and by neutron diffraction (ND, bulk region).
SXRD possesses a higher spatial resolution than ND. Magnetic stray fields were mapped by utilizing high-spatial-resolution giant magneto resistance (GMR) sensors.
Results
The subsurface residual stress overall correlates better with the magnetic stray field distribution than the bulk stress. This correlation is especially visible in the regions outside the heat affected zone, where the influence of the microstructural features is less pronounced but steep residual stress gradients are present.
Conclusions
It was demonstrated that the localized stray field sources without any obvious microstructural variations are associated with steep stress gradients.
The good correlation between subsurface residual stress and magnetic signal indicates that the source of the magnetic stray fields is to be found in the range of the penetration depth of the SXRD measurements.
Gravitational waves from the collision of binary neutron stars provide a unique opportunity to study the behaviour of supranuclear matter, the fundamental properties of gravity and the cosmic history of our Universe. However, given the complexity of Einstein's field equations, theoretical models that enable source-property inference suffer from systematic uncertainties due to simplifying assumptions. We develop a hypermodel approach to compare and measure the uncertainty of gravitational-wave approximants. Using state-of-the-art models, we apply this new technique to the binary neutron star observations GW170817 and GW190425 and to the sub-threshold candidate GW200311_103121. Our analysis reveals subtle systematic differences (with Bayesian odds of similar to 2) between waveform models. A frequency-dependence study suggests that this may be due to the treatment of the tidal sector. This new technique provides a proving ground for model development and a means to identify waveform systematics in future observing runs where detector improvements will increase the number and clarity of binary neutron star collisions we observe.
Accurate and precise characterization of cirrus cloud geometrical and optical properties is essential for better constraining their radiative footprint. A lidar-based retrieval scheme is proposed here, with its performance assessed on fine spatio-temporal observations over the Arctic site of Ny-Alesund, Svalbard. Two contributions related to cirrus geometrical (dynamic Wavelet Covariance Transform (WCT)) and optical properties (constrained Klett) are reported. The dynamic WCT rendered cirrus detection more robust, especially for thin cirrus layers that frequently remained undetected by the classical WCT method. Regarding optical characterization, we developed an iterative scheme for determining the cirrus lidar ratio (LRci) that is a crucial parameter for aerosol - cloud discrimination. Building upon the Klett-Fernald method, the LRci was constrained by an additional reference value. In established methods, such as the double-ended Klett, an aerosol-free reference value is applied. In the proposed constrained Klett, however, the reference value was approximated from cloud-free or low cloud optical depth (COD up to 0.2) profiles and proved to agree with independent Raman estimates. For optically thin cirrus, the constrained Klett inherent uncertainties reached 50% (60-74%) in terms of COD (LRci). However, for opaque cirrus COD (LRci) uncertainties were lower than 10% (15%). The detection method discrepancies (dynamic versus static WCT) had a higher impact on the optical properties of low COD layers (up to 90%) compared to optically thicker ones (less than 10%). The constrained Klett presented high agreement with two established retrievals. For an exemplary cirrus cloud, the constrained Klett estimated the COD355 (LRci355) at 0.28 +/- 0.17 (29 +/- 4 sr), the double-ended Klett at 0.27 +/- 0.15 (32 +/- 4 sr) and the Raman retrievals at 0.22 +/- 0.12 (26 +/- 11 sr). Our approach to determine the necessary reference value can also be applied in established methods and increase their accuracy. In contrast, the classical aerosol-free assumption led to 44 sr LRci overestimation in optically thin layers and 2-8 sr in thicker ones. The multiple scattering effect was corrected using Eloranta (1998) and accounted for 50-60% extinction underestimation near the cloud base and 20-30% within the cirrus layers.
We present the analysis of Very Large Telescope Multi Unit Spectroscopic Explorer (MUSE) observations of the planetary nebula (PN) IC 4406. MUSE images in key emission lines are used to unveil the presence of at least five ring-like structures north and south of the main nebula of IC4406. MUSE spectra are extracted from the rings to unambiguously assess for the first time in a PN their physical conditions, electron density (n(e)), and temperature (T-e). The rings are found to have similar T-e as the rim of the main nebula, but smaller n(e). Ratios between different ionic species suggest that the rings of IC4406 have a lower ionization state than the main cavity, in contrast to what was suggested for the rings in NGC 6543, the Cat's Eye Nebula.
The current paradigm of cosmic-ray (CR) origin states that the greater part of galactic CRs is produced by supernova remnants. The interaction of supernova ejecta with the interstellar medium after a supernova's explosions results in shocks responsible for CR acceleration via diffusive shock acceleration (DSA). We use particle-in-cell (PIC) simulations and a combined PIC-magnetohydrodynamic (PIC-MHD) technique to investigate whether DSA can occur in oblique high Mach number shocks. Using the PIC method, we follow the formation of the shock and determine the fraction of the particles that gets involved in DSA. With this result, we use PIC-MHD simulations to model the large-scale structure of the plasma and the magnetic field surrounding the shock and find out whether or not the reflected particles can generate upstream turbulence and trigger DSA. We find that the feasibility of this process in oblique shocks depends strongly on the Alfvenic Mach number, and the DSA process is more likely to be triggered at high Mach number shocks.
A detailed investigation of the energy levels of perylene-3,4,9,10-tetracarboxylic tetraethylester as a representative compound for the whole family of perylene esters was performed. It was revealed via electrochemical measurements that one oxidation and two reductions take place. The bandgaps determined via the electrochemical approach are in good agreement with the optical bandgap obtained from the absorption spectra via a Tauc plot. In addition, absorption spectra in dependence of the electrochemical potential were the basis for extensive quantum-chemical calculations of the neutral, monoanionic, and dianionic molecules. For this purpose, calculations based on density functional theory were compared with post-Hartree-Fock methods and the CAM-B3LYP functional proved to be the most reliable choice for the calculation of absorption spectra. Furthermore, spectral features found experimentally could be reproduced with vibronic calculations and allowed to understand their origins. In particular, the two lowest energy absorption bands of the anion are not caused by absorption of two distinct electronic states, which might have been expected from vertical excitation calculations, but both states exhibit a strong vibronic progression resulting in contributions to both bands.
We have analysed an archival XMM-Newton EPIC observation that serendipitously covered the sky position of a variable X-ray source AX J1714.1-3912, previously suggested to be a Supergiant Fast X-ray Transient (SFXT). During the XMM-Newton observation the source is variable on a timescale of hundred seconds and shows two luminosity states, with a flaring activity followed by unflared emission, with a variability amplitude of a factor of about 50. We have discovered an intense iron emission line with a centroid energy of 6.4 keV in the power law-like spectrum, modified by a large absorption (N-H similar to 10(24) cm(-2)), never observed before from this source. This X-ray spectrum is unusual for an SFXT, but resembles the so-called 'highly obscured sources', high mass X-ray binaries (HMXBs) hosting an evolved B[e] supergiant companion (sgB[e]). This might suggest that AX J1714.1-3912 is a new member of this rare type of HMXBs, which includes IGR J16318-4848 and CI Camelopardalis. Increasing this small population of sources would be remarkable, as they represent an interesting short transition evolutionary stage in the evolution of massive binaries. Nevertheless, AX J1714.1-3912 appears to share X-ray properties of both kinds of HMXBs (SFXT versus sgB[e] HMXB). Therefore, further investigations of the companion star are needed to disentangle the two hypothesis.
Phase equilibria that are relevant for the growth of Bi2MO4 have been studied experimentally, and the ternary phase diagrams of Bi2O3-PdO2-Pd and Bi2O3-Cu2O-CuO and its isopleth section Bi2O3-CuO were redetermined. It is shown that every melting and crystallization process is always accompanied by a redox process at the phase boundary and that for both title compounds, the valence of the transition metal is lowered during melting. Vice versa, during crystal growth, O-2 must be transported through the melt to the phase boundary. Based on these new insights provided by our thermodynamic studies, Bi2CuO4 single crystals with a length of up to 7 cm and a diameter of 6 mm were grown by the OFZ technique to be used for investigations of magnetic, electronic and thermal transport properties. The grown crystals were characterized by powder X-ray diffraction, Laue, magnetization and specific heat measurements.
Most image restoration methods in astronomy rely upon probabilistic tools that infer the best solution for a deconvolution problem. They achieve good performances when the point spread function (PSF) is spatially invariant in the image plane.
However, this condition is not always satisfied in real optical systems. We propose a new method for the restoration of images affected by static and anisotropic aberrations using Deep Neural Networks that can be directly applied to sky images.
The network is trained using simulated sky images corresponding to the T80-S Telescope optical model, a 80-cm survey imager at Cerro Tololo (Chile), which are synthesized using a Zernike polynomial representation of the optical system.
Once trained, the network can be used directly on sky images, outputting a corrected version of the image that has a constant and known PSF across its field of view. The method is to be tested on the T80-S Telescope.
We present the method and results on synthetic data.
3A 1954+319 has been classified for a long time as a symbiotic X-ray binary, hosting a slowly rotating neutron star and an aged M red giant. Recently, this classification has been revised thanks to the discovery that the donor star is an M supergiant. This makes 3A 1954+319 a rare type of high-mass X-ray binary consisting of a neutron star and a red supergiant donor. In this paper, we analyse two archival and still unpublished XMM-Newton and NuSTAR observations of the source. We perform a detailed hardness ratio-resolved spectral analysis to search for spectral variability that could help investigating the structures of the inhomogeneous M supergiant wind from which the neutron star is accreting. We discuss our results in the context of wind-fed supergiant X-ray binaries and show that the newest findings on 3A 1954+319 reinforce the hypothesis that the neutron star in this system is endowed with a magnetar-like magnetic field strength (greater than or similar to 10(14) G).
The combined effect of ultraviolet (UV) light soaking and self-assembled monolayer deposition on the work function (WF) of thin ZnO layers and on the efficiency of hole injection into the prototypical conjugated polymer poly(3-hexylthiophen-2,5-diyl) (P3HT) is systematically investigated. It is shown that the WF and injection efficiency depend strongly on the history of UV light exposure. Proper treatment of the ZnO layer enables ohmic hole injection into P3HT, demonstrating ZnO as a potential anode material for organic optoelectronic devices. The results also suggest that valid conclusions on the energy-level alignment at the ZnO/organic interfaces may only be drawn if the illumination history is precisely known and controlled. This is inherently problematic when comparing electronic data from ultraviolet photoelectron spectroscopy (UPS) measurements carried out under different or ill-defined illumination conditions.
Context. The spectroscopic class of subdwarf A-type (sdA) stars has come into focus in recent years because of their possible link to extremely low-mass white dwarfs, a rare class of objects resulting from binary evolution. Although most sdA stars are consistent with metal-poor halo main-sequence stars, the formation and evolution of a fraction of these stars are still matters of debate. Aims. The identification of photometric variability can help to put further constraints on the evolutionary status of sdA stars, in particular through the analysis of pulsations. Moreover, the binary ratio, which can be deduced from eclipsing binaries and ellipsoidal variables, is important as input for stellar models. In order to search for variability due to either binarity or pulsations in objects of the spectroscopic sdA class, we have extracted all available high precision light curves from the Kepler K2 mission.
Methods. We have performed a thorough time series analysis on all available light curves, employing three different methods. Frequencies with a signal-to-noise ratio higher than four have been used for further analysis.
Results. From the 25 targets, 13 turned out to be variables of different kinds (i.e., classical pulsating stars, ellipsoidal and cataclysmic variables, eclipsing binaries, and rotationally induced variables). For the remaining 12 objects, a variability threshold was determined.
The oxygen on Ag(111) system has been investigated with Auger electron-photoelectron coincidence spectroscopy (APECS).
The coincidence spectra between O 1s core level photoelectrons and O KLL Auger electrons have been studied together with Ag(3)d/AgM4,5NN coincidences.
We also describe the electron-electron coincidence spectrometer setup, CoESCA, consisting of two angle resolved time-of-flight spectrometers at a synchrotron light source.
Contributions from molecular oxygen and chemisorbed oxygen are assigned using the coincidence data, conclusions are drawn primarily from the O 1s/O KLL data.
The data acquisition and treatment procedure are also outlined.
The chemisorbed oxygen species observed are relevant for the catalytic ethylene oxidation.
We present a framework for systems in which diffusion-advection transport of a tracer substance in a mobile zone is interrupted by trapping in an immobile zone.
Our model unifies different model approaches based on distributed-order diffusion equations, exciton diffusion rate models, and random-walk models for multirate mobile-immobile mass transport.
We study various forms for the trapping time dynamics and their effects on the tracer mass in the mobile zone.
Moreover, we find the associated breakthrough curves, the tracer density at a fixed point in space as a function of time, and the mobile and immobile concentration profiles and the respective moments of the transport.
Specifically, we derive explicit forms for the anomalous transport dynamics and an asymptotic power-law decay of the mobile mass for a Mittag-Leffler trapping time distribution.
In our analysis we point out that even for exponential trapping time densities, transient anomalous transport is observed.
Our results have direct applications in geophysical contexts, but also in biological, soft matter, and solid state systems.
The control of residual stress (RS) remains a challenge in the manufacturing of metallic parts using the laser powder bed fusion process (LPBF). This layer-by-layer manufacturing approach gives rise to complex triaxial RS distributions, which require extensive characterization effort for a broader acceptance of LPBF in industry. This study focuses on the distribution of bulk triaxial RS and surface RS in LPBF austenitic steel 316L. The RS are determined by X-ray and neutron diffraction to characterize the RS distribution. Variations in the LPBF parameters interlayer time (ILT) and scanning velocity and their influence on the temperature distribution and resulting RS is investigated using thermographic data from in situ process monitoring. The RS in the LPBF 316L is tensile at the surface and compressive in the bulk. The RS is directly related to the thermal history of the part as shown by the in situ thermography data. Shorter ILT leads to higher temperatures of the part during the manufacturing, which decrease the RS and RS formation mechanisms. Interestingly, the surface RS does not agree with this observation. This study highlights the benefit of using multiple RS determination methods and in situ thermography monitoring to characterize the RS in LPBF processed parts.
The most complex but potentially most severe impacts of climate change are caused by extreme weather events. In a globally connected economy, damages can cause remote perturbations and cascading consequences-a ripple effect along supply chains. Here we show an economic ripple resonance that amplifies losses when consecutive or overlapping weather extremes and their repercussions interact. This amounts to an average amplification of 21% for climate-induced heat stress, river floods, and tropical cyclones. Modeling the temporal evolution of 1.8 million trade relations between >7000 regional economic sectors, we find that the regional responses to future extremes are strongly heterogeneous also in their resonance behavior. The induced effect on welfare varies between gains due to increased demand in some regions and losses due to demand or supply shortages in others. Within the current global supply network, the ripple resonance effect of extreme weather is strongest in high-income economies-an important effect to consider when evaluating past and future economic climate impacts.
Visible light is shown to create a transient metallic S-Mo-S surface layer on bulk semiconducting p-doped indirect-bandgap 2H-MoS2. Optically created electron-hole pairs separate in the surface band bending region of the p-doped semiconducting crystal causing a transient accumulation of electrons in the surface region. This triggers a reversible 2H-semiconductor to 1T-metal phase-transition of the surface layer. Electron-phonon coupling of the indirect-bandgap p-doped 2H-MoS2 enables this efficient pathway even at a low density of excited electrons with a distinct optical excitation threshold and saturation behavior. This mechanism needs to be taken into consideration when describing the surface properties of illuminated p-doped 2H-MoS2. In particular, light-induced increased charge mobility and surface activation can cause and enhance the photocatalytic and photoassisted electrochemical hydrogen evolution reaction of water on 2H-MoS2. Generally, it opens up for a way to control not only the surface of p-doped 2H-MoS2 but also related dichalcogenides and layered systems. The findings are based on the sensitivity of time-resolved electron spectroscopy for chemical analysis with photon-energy-tuneable synchrotron radiation.
The enhancement and control of the electrical conductivity of organic semiconductors is fundamental for their use in optoelectronic applications and can be achieved by molecular doping, which introduces additional charge carriers through electron transfer between a dopant molecule and the organic semiconductor. Here, we use Electron Paramagnetic Resonance (EPR) spectroscopy to characterise the unpaired spins associated with the charges generated by molecular doping of the prototypical organic semiconductor poly(3-hexylthiophene) (P3HT) with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F(4)TCNQ) and tris(pentafluorophenyl)borane (BCF). The EPR results reveal the P3HT radical cation as the only paramagnetic species in BCF-doped P3HT films and show evidence for increased mobility of the detected spins at high doping concentrations as well as formation of antiferromagnetically coupled spin pairs leading to decreased spin concentrations at low temperatures. The EPR signature for F(4)TCNQ-doped P3HT is found to be determined by spin exchange between P3HT radical cations and F(4)TCNQ radical anions. Results from continuous-wave and pulse EPR measurements suggest the presence of the unpaired spin on P3HT in a multitude of environments, ranging from free P3HT radical cations with similar properties to those observed in BCF-doped P3HT, to pairs of dipolar and exchange-coupled spins on P3HT and the dopant anion. Characterisation of the proton hyperfine interactions by ENDOR allowed quantification of the extent of spin delocalisation and revealed reduced delocalisation in the F(4)TCNQ-doped P3HT films.
We study a heterogeneous diffusion process (HDP) with position-dependent diffusion coefficient and Poissonian stochastic resetting.
We find exact results for the mean squared displacement and the probability density function. The nonequilibrium steady state reached in the long time limit is studied.
We also analyse the transition to the non-equilibrium steady state by finding the large deviation function.
We found that similarly to the case of the normal diffusion process where the diffusion length grows like t (1/2) while the length scale xi(t) of the inner core region of the nonequilibrium steady state grows linearly with time t, in the HDP with diffusion length increasing like t ( p/2) the length scale xi(t) grows like t ( p ).
The obtained results are verified by numerical solutions of the corresponding Langevin equation.
Here we show that microgels trapped at a solid wall can issue liquid flow and transport over distances several times larger than the particle size.
The microgel consists of cross-linked poly(N-isopropylacrylamide-co-acrylic acid) (PNIPAM-AA) polymer chains loaded with cationic azobenzene-containing surfactant, which can assume either a trans-or a cis-state depending on the wavelength of the applied irradiation. The microgel, being a selective absorber of trans-isomers, responds by changing its volume under irradiation with light of appropriate wavelength at which the cis-isomers of the surfactant molecules diffuse out of the particle interior.
Together with the change in particle size, the expelled cis-isomers form an excess of the concentration and subsequent gradient in osmotic pressure generating a halo of local light-driven diffusioosmotic (l-LDDO) flow. The direction and the strength of the l-LDDO depends on the intensity and irradiation wavelength, as well as on the amount of surfactant absorbed by the microgel.
The flow pattern around a microgel is directed radially outward and can be maintained quasi-indefinitely under exposure to blue light when the trans-/cis-ratio is 2/1, establishing a photostationary state.
Irradiation with UV light, on the other hand, generates a radially transient flow pattern, which inverts from inward to outward over time at low intensities.
By measuring the displacement of tracer particles around neutral microgels during a temperature-induced collapse, we can exclude that a change in particle shape itself causes the flow, i.e., just by expulsion or uptake of water.
Ultimately, it is its ability to selectively absorb two isomers of photosensitive surfactant under different irradiation conditions that leads to an effective pumping caused by a self-induced diffusioosmotic flow.
Symmetry and its breaking crucially define the chemical properties of molecules and their functionality. Resonant inelastic X-ray scattering is a local electronic structure probe reporting on molecular symmetry and its dynamical breaking within the femtosecond scattering duration. Here, we study pyrimidine, a system from the C-2v point group, in an aqueous solution environment, using scattering though its 2a(2) resonance. Despite the absence of clean parity selection rules for decay transitions from in-plane orbitals, scattering channels including decay from the 7b(2) and 11a(1) orbitals with nitrogen lone pair character are a direct probe for molecular symmetry. Computed spectra of explicitly solvated molecules sampled from a molecular dynamics simulation are combined with the results of a quantum dynamical description of the X-ray scattering process. We observe dominant signatures of core-excited Jahn-Teller induced symmetry breaking for resonant excitation. Solvent contributions are separable by shortening of the effective scattering duration through excitation energy detuning.
Based on suggested interactions of potential tipping elements in the Earth's climate and in ecological systems, tipping cascades as possible dynamics are increasingly discussed and studied. The activation of such tipping cascades would impose a considerable risk for human societies and biosphere integrity. However, there are ambiguities in the description of tipping cascades within the literature so far. Here we illustrate how different patterns of multiple tipping dynamics emerge from a very simple coupling of two previously studied idealized tipping elements. In particular, we distinguish between a two phase cascade, a domino cascade and a joint cascade. A mitigation of an unfolding two phase cascade may be possible and common early warning indicators are sensitive to upcoming critical transitions to a certain degree. In contrast, a domino cascade may hardly be stopped once initiated and critical slowing down-based indicators fail to indicate tipping of the following element. These different potentials for intervention and anticipation across the distinct patterns of multiple tipping dynamics should be seen as a call to be more precise in future analyses of cascading dynamics arising from tipping element interactions in the Earth system.
This paper studies cosmic-ray (CR) transport in magnetohydrodynamic (MHD) turbulence. CR transport is strongly dependent on the properties of the magnetic turbulence.
We perform test particle simulations to study the interactions of CR with both total MHD turbulence and decomposed MHD modes.
The spatial diffusion coefficients and the pitch angle scattering diffusion coefficients are calculated from the test particle trajectories in turbulence.
Our results confirm that the fast modes dominate the CR propagation, whereas Alfven and slow modes are much less efficient and have shown similar pitch-angle scattering rates.
We investigate the cross field transport on large and small scales. On large/global scales, normal diffusion is observed and the diffusion coefficient is suppressed by M-A(zeta) compared to the parallel diffusion coefficients, with zeta closer to 4 in Alfven modes than that in total turbulence, as theoretically expected.
For the CR transport on scales smaller than the turbulence injection scale, both the local and global magnetic reference frames are adopted. Superdiffusion is observed on such small scales in all the cases. Particularly, CR transport in Alfven modes show clear Richardson diffusion in the local reference frame. The diffusion transitions smoothly from the Richardson's one with index 1.5 to normal diffusion as the particle mean free path decreases from lambda(parallel to) >> L to lambda(parallel to) << L, where L is the injection/coherence length of turbulence.
Our results have broad applications to CRs in various astrophysical environments.
Active matter broadly covers the dynamics of self-propelled particles.
While the onset of collective behavior in homogenous active systems is relatively well understood, the effect of inhomogeneities such as obstacles and traps lacks overall clarity.
Here, we study how interacting, self-propelled particles become trapped and released from a trap.
We have found that captured particles aggregate into an orbiting condensate with a crystalline structure. As more particles are added, the trapped condensates escape as a whole.
Our results shed light on the effects of confinement and quenched disorder in active matter.
Cirrus is the only cloud type capable of inducing daytime cooling or heating at the top of the atmosphere (TOA) and the sign of its radiative effect highly depends on its optical depth. However, the investigation of its geometrical and optical properties over the Arctic is limited. In this work the long-term properties of cirrus clouds are explored for the first time over an Arctic site (Ny-Alesund, Svalbard) using lidar and radiosonde measurements from 2011 to 2020. The optical properties were quality assured, taking into account the effects of specular reflections and multiple-scattering. Cirrus clouds were generally associated with colder and calmer wind conditions compared to the 2011-2020 climatology. However, the dependence of cirrus properties on temperature and wind speed was not strong. Even though the seasonal cycle was not pronounced, the winter-time cirrus appeared under lower temperatures and stronger wind conditions. Moreover, in winter, geometrically- and optically-thicker cirrus were found and their ice particles tended to be more spherical. The majority of cirrus was associated with westerly flow and westerly cirrus tended to be geometrically-thicker. Overall, optically-thinner layers tended to comprise smaller and less spherical ice crystals, most likely due to reduced water vapor deposition on the particle surface. Compared to lower latitudes, the cirrus layers over Ny-Alesund were more absorbing in the visible spectral region and they consisted of more spherical ice particles.
Complex networks are abundant in nature and many share an important structural property: they contain a few nodes that are abnormally highly connected (hubs). Some of these hubs are called influencers because they couple strongly to the network and play fundamental dynamical and structural roles. Strikingly, despite the abundance of networks with influencers, little is known about their response to stochastic forcing. Here, for oscillatory dynamics on influencer networks, we show that subjecting influencers to an optimal intensity of noise can result in enhanced network synchronization. This new network dynamical effect, which we call coherence resonance in influencer networks, emerges from a synergy between network structure and stochasticity and is highly nonlinear, vanishing when the noise is too weak or too strong. Our results reveal that the influencer backbone can sharply increase the dynamical response in complex systems of coupled oscillators. Influencer networks include a small set of highly-connected nodes and can reach synchrony only via strong node interaction. Tonjes et al. show that introducing an optimal amount of noise enhances synchronization of such networks, which may be relevant for neuroscience or opinion dynamics applications.
The mean free path of ionizing photons, lambda(mfp), is a key factor in the photoionization of the intergalactic medium (IGM). At z greater than or similar to 5, however, lambda(mfp) may be short enough that measurements towards QSOs are biased by the QSO proximity effect. We present new direct measurements of lambda(mfp) that address this bias and extend up to z similar to 6 for the first time. Our measurements at z similar to 5 are based on data from the Giant Gemini GMOS survey and new Keck LRIS observations of low-luminosity QSOs. At z similar to 6 we use QSO spectra from Keck ESI and VLT X-Shooter. We measure lambda(mfp) = 9.09(-1.28)(+1.62) proper Mpc and 0.75(-0.45)(+0.65) proper Mpc (68 percent confidence) at z = 5.1 and 6.0, respectively. The results at z = 5.1 are consistent with existing measurements, suggesting that bias from the proximity effect is minor at this redshift. At z = 6.0, however, we find that neglecting the proximity effect biases the result high by a factor of two or more. Our measurement at z = 6.0 falls well below extrapolations from lower redshifts, indicating rapid evolution in lambda(mfp) over 5 < z < 6. This evolution disfavours models in which reionization ended early enough that the IGM had time to fully relax hydrodynamically by z = 6, but is qualitatively consistent with models wherein reionization completed at z = 6 or even significantly later. Our mean free path results are most consistent with late reionization models wherein the IGM is still 20 percent neutral at z = 6, although our measurement at z = 6.0 is even lower than these models prefer.
In contrast to the common conception that the interfacial energy-level alignment is affixed once the interface is formed, we demonstrate that heterojunctions between organic semiconductors and metal-halide perovskites exhibit huge energy-level realignment during photoexcitation. Importantly, the photoinduced level shifts occur in the organic component, including the first molecular layer in direct contact with the perovskite. This is caused by charge-carrier accumulation within the organic semiconductor under illumination and the weak electronic coupling between the junction components.
Surface melting of the Greenland Ice Sheet contributes a large amount to current and future sea level rise. Increased surface melt may lower the reflectivity of the ice sheet surface and thereby increase melt rates: the so-called melt-albedo feedback describes this self-sustaining increase in surface melting. In order to test the effect of the melt-albedo feedback in a prognostic ice sheet model, we implement dEBM-simple, a simplified version of the diurnal Energy Balance Model dEBM, in the Parallel Ice Sheet Model (PISM). The implementation includes a simple representation of the melt-albedo feedback and can thereby replace the positive-degree-day melt scheme. Using PISM-dEBM-simple, we find that this feedback increases ice loss through surface warming by 60 % until 2300 for the high-emission scenario RCP8.5 when compared to a scenario in which the albedo remains constant at its present-day values. With an increase of 90 % compared to a fixed-albedo scenario, the effect is more pronounced for lower surface warming under RCP2.6. Furthermore, assuming an immediate darkening of the ice surface over all summer months, we estimate an upper bound for this effect to be 70 % in the RCP8.5 scenario and a more than 4-fold increase under RCP2.6. With dEBM-simple implemented in PISM, we find that the melt-albedo feedback is an essential contributor to mass loss in dynamic simulations of the Greenland Ice Sheet under future warming.
Predicting the electron population of Earth's ring current during geomagnetic storms still remains a challenging task.
In this work, we investigate the sensitivity of 10 keV ring current electrons to different driving processes, parameterised by the Kp index, during several moderate and intense storms.
Results are validated against measurements from the Van Allen Probes satellites. Perturbing the Kp index allows us to identify the most dominant processes for moderate and intense storms respectively.
We find that during moderate storms (Kp < 6) the drift velocities mostly control the behaviour of low energy electrons, while loss from wave-particle interactions is the most critical parameter for quantifying the evolution of intense storms (Kp > 6). Perturbations of the Kp index used to drive the boundary conditions at GEO and set the plasmapause location only show a minimal effect on simulation results over a limited L range.
It is further shown that the flux at L & SIM; 3 is more sensitive to changes in the Kp index compared to higher L shells, making it a good proxy for validating the source-loss balance of a ring current model.
Motivated by recent epidemic outbreaks, including those of COVID-19, we solve the canonical problem of calculating the dynamics and likelihood of extensive outbreaks in a population within a large class of stochastic epidemic models with demographic noise, including the susceptible-infected-recovered (SIR) model and its general extensions.
In the limit of large populations, we compute the probability distribution for all extensive outbreaks, including those that entail unusually large or small (extreme) proportions of the population infected.
Our approach reveals that, unlike other well-known examples of rare events occurring in discrete-state stochastic systems, the statistics of extreme outbreaks emanate from a full continuum of Hamiltonian paths, each satisfying unique boundary conditions with a conserved probability flux.
Symbiotic X-ray binaries are systems hosting a neutron star accreting form the wind of a late-type companion. These are rare objects and so far only a handful of them are known. One of the most puzzling aspects of the symbiotic X-ray binaries is the possibility that they contain strongly magnetized neutron stars. These are expected to be evolutionary much younger compared to their evolved companions and could thus be formed through the (yet poorly known) accretion induced collapse of a white dwarf. In this paper, we perform a broad-band X-ray and soft gamma-ray spectroscopy of two known symbiotic binaries, Sct X-1 and 4U 1700+24, looking for the presence of cyclotron scattering features that could confirm the presence of strongly magnetized NSs. We exploited available Chandra, Swift, and NuSTAR data. We find no evidence of cyclotron resonant scattering features (CRSFs) in the case of Sct X-1 but in the case of 4U 1700+24 we suggest the presence of a possible CRSF at similar to 16 keV and its first harmonic at similar to 31 keV, although we could not exclude alternative spectral models for the broad-band fit. If confirmed by future observations, 4U 1700+24 could be the second symbiotic X-ray binary with a highly magnetized accretor. We also report about our long-term monitoring of the last discovered symbiotic X-ray binary IGR J17329-2731 performed with Swift/XRT. The monitoring revealed that, as predicted, in 2017 this object became a persistent and variable source, showing X-ray flares lasting for a few days and intriguing obscuration events that are interpreted in the context of clumpy wind accretion.
Non-fullerene acceptors (NFAs) are far more emissive than their fullerene-based counterparts. Here, we study the spectral properties of photocurrent generation and recombination of the blend of the donor polymer PM6 with the NFA Y6. We find that the radiative recombination of free charges is almost entirely due to the re-occupation and decay of Y6 singlet excitons, but that this pathway contributes less than 1% to the total recombination. As such, the open-circuit voltage of the PM6:Y6 blend is determined by the energetics and kinetics of the charge-transfer (CT) state. Moreover, we find that no information on the energetics of the CT state manifold can be gained from the low-energy tail of the photovoltaic external quantum efficiency spectrum, which is dominated by the excitation spectrum of the Y6 exciton. We, finally, estimate the charge-separated state to lie only 120 meV below the Y6 singlet exciton energy, meaning that this blend indeed represents a high-efficiency system with a low energetic offset.
The first detections of black hole-neutron star mergers (GW200105 and GW200115) by the LIGO-Virgo-Kagra Collaboration mark a significant scientific breakthrough. The physical interpretation of pre- and postmerger signals requires careful cross-examination between observational and theoretical modelling results. Here we present the first set of black hole-neutron star simulations that were obtained with the numerical-relativity code BAM. Our initial data are constructed using the public LORENE spectral library, which employs an excision of the black hole interior. BAM, in contrast, uses the moving-puncture gauge for the evolution. Therefore, we need to "stuff" the black hole interior with smooth initial data to evolve the binary system in time. This procedure introduces constraint violations such that the constraint damping properties of the evolution system are essential to increase the accuracy of the simulation and in particular to reduce spurious center-of-mass drifts. Within BAM we evolve the Z4c equations and we compare our gravitational-wave results with those of the SXS collaboration and results obtained with the SACRA code. While we find generally good agreement with the reference solutions and phase differences less than or similar to 0.5 rad at the moment of merger, the absence of a clean convergence order in our simulations does not allow for a proper error quantification. We finally present a set of different initial conditions to explore how the merger of black hole neutron star systems depends on the involved masses, spins, and equations of state.
The nature of the sources powering nebular He II emission in star-forming galaxies remains debated, and various types of objects have been considered, including Wolf-Rayet stars, X-ray binaries, and Population III stars.
Modern X-ray observations show the ubiquitous presence of hot gas filling star-forming galaxies. We use a collisional ionization plasma code to compute the specific He II ionizing flux produced by hot gas and show that if its temperature is not too high (less than or similar to 2.5 MK), then the observed levels of soft diffuse X-ray radiation could explain He II ionization in galaxies.
To gain a physical understanding of this result, we propose a model that combines the hydrodynamics of cluster winds and hot superbubbles with observed populations of young massive clusters in galaxies. We find that in low-metallicity galaxies, the temperature of hot gas is lower and the production rate of He II ionizing photons is higher compared to high-metallicity galaxies. The reason is that the slower stellar winds of massive stars in lower-metallicity galaxies input less mechanical energy in the ambient medium.
Furthermore, we show that ensembles of star clusters up to similar to 10-20 Myr old in galaxies can produce enough soft X-rays to induce nebular He II emission. We discuss observations of the template low-metallicity galaxy I Zw 18 and suggest that the He II nebula in this galaxy is powered by a hot superbubble.
Finally, appreciating the complex nature of stellar feedback, we suggest that soft X-rays from hot superbubbles are among the dominant sources of He II ionizing flux in low-metallicity star-forming galaxies.
Starting from the observation that the reduced state of a system strongly coupled to a bath is, in general, an athermal state, we introduce and study a cyclic battery-charger quantum device that is in thermal equilibrium, or in a ground state, during the charge storing stage. The cycle has four stages: the equilibrium storage stage is interrupted by disconnecting the battery from the charger, then work is extracted from the battery, and then the battery is reconnected with the charger; finally, the system is brought back to equilibrium. At no point during the cycle are the battery-charger correlations artificially erased. We study the case where the battery and charger together comprise a spin-1/2 Ising chain, and show that the main characteristics-the extracted energy and the thermodynamic efficiency-can be enhanced by operating the cycle close to the quantum phase transition point. When the battery is just a single spin, we find that the output work and efficiency show a scaling behavior at criticality and derive the corresponding critical exponents. Due to always present correlations between the battery and the charger, operations that are equivalent from the perspective of the battery can entail different energetic costs for switching the battery-charger coupling. This happens only when the coupling term does not commute with the battery's bare Hamiltonian, and we use this purely quantum leverage to further optimize the performance of the device.
The influence of the process gas, laser scan speed, and sample thickness on the build-up of residual stresses and porosity in Ti-6Al-4V produced by laser powder bed fusion was studied. Pure argon and helium, as well as a mixture of those (30% helium), were employed to establish process atmospheres with a low residual oxygen content of 100 ppm O-2. The results highlight that the subsurface residual stresses measured by X-ray diffraction were significantly lower in the thin samples (220 MPa) than in the cuboid samples (645 MPa). This difference was attributed to the shorter laser vector length, resulting in heat accumulation and thus in-situ stress relief. The addition of helium to the process gas did not introduce additional subsurface residual stresses in the simple geometries, even for the increased scanning speed. Finally, larger deflection was found in the cantilever built under helium (after removal from the baseplate), than in those produced under argon and an argon-helium mixture. This result demonstrates that complex designs involving large scanned areas could be subjected to higher residual stress when manufactured under helium due to the gas's high thermal conductivity, heat capacity, and thermal diffusivity.
Enhanced charge selectivity via anodic-C60 layer reduces nonradiative losses in organic solar cells
(2021)
Interfacial layers in conjunction with suitable charge-transport layers can significantly improve the performance of optoelectronic devices by facilitating efficient charge carrier injection and extraction.
This work uses a neat C-60 interlayer on the anode to experimentally reveal that surface recombination is a significant contributor to nonradiative recombination losses in organic solar cells.
These losses are shown to proportionally increase with the extent of contact between donor molecules in the photoactive layer and a molybdenum oxide (MoO3) hole extraction layer, proven by calculating voltage losses in low- and high-donor-content bulk heterojunction device architectures.
Using a novel in-device determination of the built-in voltage, the suppression of surface recombination, due to the insertion of a thin anodic-C-60 interlayer on MoO3, is attributed to an enhanced built-in potential.
The increased built-in voltage reduces the presence of minority charge carriers at the electrodes-a new perspective on the principle of selective charge extraction layers.
The benefit to device efficiency is limited by a critical interlayer thickness, which depends on the donor material in bilayer devices.
Given the high popularity of MoO3 as an efficient hole extraction and injection layer and the increasingly popular discussion on interfacial phenomena in organic optoelectronic devices, these findings are relevant to and address different branches of organic electronics, providing insights for future device design.
The addition of nano-Al2O3 has been shown to enhance the breakdown voltage of epoxy resin, but its flashover results appeared with disputation. This work concentrates on the surface charge variation and dc flashover performance of epoxy resin with nano-Al2O3 doping. The dispersion of nano-Al2O3 in epoxy is characterized by scanning electron microscopy (SEM) and atomic force microscopy (AFM). The dc flashover voltages of samples under either positive or negative polarity are measured with a finger-electrode system, and the surface charge variations before and after flashovers were identified from the surface potential mapping. The results evidence that nano-Al2O3 would lead to a 16.9% voltage drop for the negative flashovers and a 6.8% drop for positive cases. It is found that one-time flashover clears most of the accumulated surface charges, regardless of positive or negative. As a result, the ground electrode is neighbored by an equipotential zone enclosed with low-density heterocharges. The equipotential zone tends to be broadened after 20 flashovers. The nano-Al2O3 is noticed as beneficial to downsize the equipotential zone due to its capability on charge migration, which is reasonable to maintain flashover voltage at a high level after multiple flashovers. Hence, nano-Al2O3 plays a significant role in improving epoxy with high resistance to multiple flashovers.
R-Group stabilization in methylated formamides observed by resonant inelastic X-ray scattering
(2022)
The inherent stability of methylated formamides is traced to a stabilization of the deep-lying sigma-framework by resonant inelastic X-ray scattering at the nitrogen K-edge. Charge transfer from the amide nitrogen to the methyl groups underlie this stabilization mechanism that leaves the aldehyde group essentially unaltered and explains the stability of secondary and tertiary amides.