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Young core-collapse supernovae with dense-wind progenitors may be able to accelerate cosmic-ray hadrons beyond the knee of the cosmic-ray spectrum, and this may result in measurable gamma-ray emission. We searched for gamma-ray emission from ten super- novae observed with the High Energy Stereoscopic System (H.E.S.S.) within a year of the supernova event. Nine supernovae were observed serendipitously in the H.E.S.S. data collected between December 2003 and December 2014, with exposure times ranging from 1.4 to 53 h. In addition we observed SN 2016adj as a target of opportunity in February 2016 for 13 h. No significant gamma-ray emission has been detected for any of the objects, and upper limits on the >1 TeV gamma-ray flux of the order of similar to 10(-13) cm(-)(2)s(-1) are established, corresponding to upper limits on the luminosities in the range similar to 2 x 10(39) to similar to 1 x 10(42) erg s(-1). These values are used to place model-dependent constraints on the mass-loss rates of the progenitor stars, implying upper limits between similar to 2 x 10(-5) and similar to 2 x 10(-3) M-circle dot yr(-1) under reasonable assumptions on the particle acceleration parameters.
Femtosecond x-ray diffraction reveals a liquid-liquid phase transition in phase-change materials
(2019)
In phase-change memory devices, a material is cycled between glassy and crystalline states. The highly temperature-dependent kinetics of its crystallization process enables application in memory technology, but the transition has not been resolved on an atomic scale. Using femtosecond x-ray diffraction and ab initio computer simulations, we determined the time-dependent pair-correlation function of phase-change materials throughout the melt-quenching and crystallization process. We found a liquid-liquid phase transition in the phase-change materials Ag4In3Sb67Te26 and Ge15Sb85 at 660 and 610 kelvin, respectively. The transition is predominantly caused by the onset of Peierls distortions, the amplitude of which correlates with an increase of the apparent activation energy of diffusivity. This reveals a relationship between atomic structure and kinetics, enabling a systematic optimization of the memory-switching kinetics.
We report on a combined theoretical and experimental study of core-excitation spectra of gas and liquid phase methanol as obtained with the use of X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). The electronic transitions are studied with computational methods that include strict and extended second-order algebraic diagrammatic construction [ADC(2) and ADC(2)-x], restricted active space second-order perturbation theory, and time-dependent density functional theory-providing a complete assignment of the near oxygen K-edge XAS. We show that multimode nuclear dynamics is of crucial importance for explaining the available experimental XAS and RIXS spectra. The multimode nuclear motion was considered in a recently developed "mixed representation" where dissociative states and highly excited vibrational modes are accurately treated with a time-dependent wave packet technique, while the remaining active vibrational modes are described using Franck-Condon amplitudes. Particular attention is paid to the polarization dependence of RIXS and the effects of the isotopic substitution on the RIXS profile in the case of dissociative core-excited states. Our approach predicts the splitting of the 2a RIXS peak to be due to an interplay between molecular and pseudo-atomic features arising in the course of transitions between dissociative core- and valence-excited states. The dynamical nature of the splitting of the 2a peak in RIXS of liquid methanol near pre-edge core excitation is shown. The theoretical results are in good agreement with our liquid phase measurements and gas phase experimental data available from the literature. (C) 2019 Author(s).
While extensive work has been dedicated to the measurement of the demagnetization time following an ultra-short laser pulse, experimental studies of its underlying microscopic mechanisms are still scarce. In transition metal ferromagnets, one of the main mechanism is the spin-flip of conduction electrons driven by electron-phonon scattering. Here, we present an original experimental method to monitor the electron-phonon mediated spin-flip scattering rate in nickel through the stringent atomic symmetry selection rules of x-ray emission spectroscopy. Increasing the phonon population leads to a waning of the 3d -> 2p(3/2) decay peak intensity, which reflects an increase of the angular momentum transfer scattering rate attributed to spin-flip. We find a spin relaxation time scale in the order of 50 fs in the 3d-band of nickel at room temperature, while consistantly, no such peak evolution is observed for the diamagnetic counterexample copper, using the same method.
Recent observations and ice-dynamic modeling suggest that a marine ice-sheet instability (MISI) might have been triggered in West Antarctica. The corresponding outlet glaciers, Pine Island Glacier (PIG) and Thwaites Glacier (TG), showed significant retreat during at least the last 2 decades. While other regions in Antarctica have the topographic predisposition for the same kind of instability, it is so far unclear how fast these instabilities would unfold if they were initiated. Here we employ the concept of similitude to estimate the characteristic timescales of several potentially MISI-prone outlet glaciers around the Antarctic coast. Our results suggest that TG and PIG have the fastest response time of all investigated outlets, with TG responding about 1.25 to 2 times as fast as PIG, while other outlets around Antarctica would be up to 10 times slower if destabilized. These results have to be viewed in light of the strong assumptions made in their derivation. These include the absence of ice-shelf buttressing, the one-dimensionality of the approach and the uncertainty of the available data. We argue however that the current topographic situation and the physical conditions of the MISI-prone outlet glaciers carry the information of their respective timescale and that this information can be partially extracted through a similitude analysis.
The tremendous success of metal-halide perovskites, especially in the field of photovoltaics, has triggered a substantial number of studies in understanding their optoelectronic properties. However, consensus regarding the electronic properties of these perovskites is lacking due to a huge scatter in the reported key parameters, such as work function (Φ) and valence band maximum (VBM) values. Here, we demonstrate that the surface photovoltage (SPV) is a key phenomenon occurring at the perovskite surfaces that feature a non-negligible density of surface states, which is more the rule than an exception for most materials under study. With ultraviolet photoelectron spectroscopy (UPS) and Kelvin probe, we evidence that even minute UV photon fluxes (500 times lower than that used in typical UPS experiments) are sufficient to induce SPV and shift the perovskite Φ and VBM by several 100 meV compared to dark. By combining UV and visible light, we establish flat band conditions (i.e., compensate the surface-state-induced surface band bending) at the surface of four important perovskites, and find that all are p-type in the bulk, despite a pronounced n-type surface character in the dark. The present findings highlight that SPV effects must be considered in all surface studies to fully understand perovskites’ photophysical properties.
Charge extraction in organic solar cells (OSCs) is commonly believed to be limited by bimolecular recombination of photogenerated charges. However, the fill factor of OSCs is usually almost entirely governed by recombination processes that scale with the first order of the light intensity. This linear loss was often interpreted to be a consequence of geminate or trap-assisted recombination. Numerical simulations show that this linear dependence is a direct consequence of the large amount of excess dark charge near the contact. The first-order losses increase with decreasing mobility of minority carriers, and we discuss the impact of several material and device parameters on this loss mechanism. This work highlights that OSCs are especially vulnerable to injected charges as a result of their poor charge transport properties. This implies that dark charges need to be better accounted for when interpreting electro-optical measurements and charge collection based on simple figures of merit.
Aims. We investigated the ionisation conditions and distances of Galactic high-velocity clouds (HVCs) in the Galactic halo and beyond in the direction of the Local Group (LG) barycentre and anti-barycentre, by studying spectral data of 29 extragalactic background sources obtained with the Cosmic Origins Spectropgraph (COS) installed on the Hubble Space Telescope (HST). Methods. We model column-densities of low, intermediate, and high ions such as Si ii, C ii, Si iii, Si vi, and C iv, and use these data to construct a set of Cloudy ionisation models. Results. In total, we found 69 high-velocity absorption components along the 29 lines of sight. The components in the direction of the LG barycentre span the entire range of studied velocities, 100 less than or similar to vertical bar nu(LSR)vertical bar less than or similar to 400 km s(-1), while those in the anti-barycentre sample have velocities up to about 300 km s(-1). For 49 components, we infer the gas densities. In the direction of the LG barycentre, the gas densities exhibit a wide range from log nH = -3.96 to -2.55, while in the anti-barycentre direction the densities are systematically higher, log nH > -3.25. The barycentre absorbers can be split into two groups based on their density: a high-density group with log nH > -3.54, which can be affected by the Milky Way radiation field, and a low-density group (log nH <= -3.54). The latter has very low thermal pressures of P/k < 7.3 Kcm(-3). Conclusions. Our study shows that part of the absorbers in the LG barycentre direction trace gas at very low gas densities and thermal pressures. These properties indicate that the absorbers are located beyond the virial radius of the Milky Way. Our study also confirms results from earlier, single-sightline studies, suggesting the presence of a metal-enriched intragroup medium filling the LG near its barycentre.
PKS 1830-211 is a known macrolensed quasar located at a redshift of z = 2.5. Its highenergy gamma-ray emission has been detected with the Fermi-Large Area Telescope (LAT) instrument and evidence for lensing was obtained by several authors from its high-energy data. Observations of PKS 1830-211 were taken with the High Energy Stereoscopic System (H.E.S.S.) array of Imaging Atmospheric Cherenkov Telescopes in 2014 August, following a flare alert by the Fermi-LAT Collaboration. The H.E.S.S observations were aimed at detecting a gamma-ray flare delayed by 20-27 d from the alert flare, as expected from observations at other wavelengths. More than 12 h of good-quality data were taken with an analysis threshold of similar to 67 GeV. The significance of a potential signal is computed as a function of the date and the average significance over the whole period. Data are compared to simultaneous observations by Fermi-LAT. No photon excess or significant signal is detected. An upper limit on PKS 1830-211 flux above 67 GeV is computed and compared to the extrapolation of the Fermi-LAT flare spectrum.
We consider collective dynamics in the ensemble of serially connected spin-torque oscillators governed by the Landau-Lifshitz-Gilbert-Slonczewski magnetization equation. Proximity to homoclinicity hampers synchronization of spin-torque oscillators: when the synchronous ensemble experiences the homoclinic bifurcation, the growth rate per oscillation of small deviations from the ensemble mean diverges. Depending on the configuration of the contour, sufficiently strong common noise, exemplified by stochastic oscillations of the current through the circuit, may suppress precession of the magnetic field for all oscillators. We derive the explicit expression for the threshold amplitude of noise, enabling this suppression.
Two new hole selective materials (HSMs) based on dangling methylsulfanyl groups connected to the C-9 position of the fluorene core are synthesized and applied in perovskite solar cells. Being structurally similar to a half of Spiro-OMeTAD molecule, these HSMs (referred as FS and DFS) share similar redox potentials but are endowed with slightly higher hole mobility, due to the planarity and large extension of their structure. Competitive power conversion efficiency (up to 18.6%) is achieved by using the new HSMs in suitable perovskite solar cells. Time-resolved photoluminescence decay measurements and electrochemical impedance spectroscopy show more efficient charge extraction at the HSM/perovskite interface with respect to Spiro-OMeTAD, which is reflected in higher photocurrents exhibited by DFS/FS-integrated perovskite solar cells. Density functional theory simulations reveal that the interactions of methylammonium with methylsulfanyl groups in DFS/FS strengthen their electrostatic attraction with the perovskite surface, providing an additional path for hole extraction compared to the sole presence of methoxy groups in Spiro-OMeTAD. Importantly, the low-cost synthesis of FS makes it significantly attractive for the future commercialization of perovskite solar cells.
There is evidence that a self-sustaining ice discharge from the West Antarctic Ice Sheet (WAIS) has started, potentially leading to its disintegration. The associated sea level rise of more than 3m would pose a serious challenge to highly populated areas including metropolises such as Calcutta, Shanghai, New York City, and Tokyo. Here, we show that the WAIS may be stabilized through mass deposition in coastal regions around Pine Island and Thwaites glaciers. In our numerical simulations, a minimum of 7400 Gt of additional snowfall stabilizes the flow if applied over a short period of 10 years onto the region (-2 mm year(-1) sea level equivalent). Mass deposition at a lower rate increases the intervention time and the required total amount of snow. We find that the precise conditions of such an operation are crucial, and potential benefits need to be weighed against environmental hazards, future risks, and enormous technical challenges.
In addition to (bacterio)chlorophylls, (B)Chls, light-harvesting complexes (LHCs) bind carotenoids, and/or their oxygen derivatives, xanthophylls. Xanthophylls/carotenoids have pivotal functions in LHCs: in stabilization of the structure, as accessory light-harvesting pigments and, probably most importantly, in photoprotection. Xanthophylls are assumed to be involved in the not yet fully understood mechanism of energy-dependent (qE) non-photochemical quenching of Chl fluorescence (NPQ) in higher plants and algae. The so called "xanthophyll cycle" appears to be crucial in this regard. The molecular mechanism(s) of xanthophyll involvement in qE/NPQ have not been established, yet. Moreover, excitation energy transfer (EET) processes involving carotenoids are also difficult to study, due to the fact that transitions between the ground state (S-0, 1(1)A(g)(-)) and the lowest excited singlet state (S-1, 2(1)A(g)(-)) of carotenoids are optically one-photon forbidden ("dark"). Two-photon excitation spectroscopic techniques have been used for more than two decades to study one-photon forbidden states of carotenoids. In the current study, two-photon excitation profiles of LHCII samples containing different xanthophyll complements were measured in the presumed 1(1)A(g)(-) -> 2(1)A(g)(-) (S-0 -> S-1) transition spectral region of the xanthophylls, as well as for isolated chlorophylls a and b in solution. The results indicate that direct two-photon excitation of Chls in this spectral region is dominant over that by xanthophylls. Implications of the results for proposed mechanism(s) of qE/NPQ will be discussed.
In magnetized plasmas such as the ionosphere, electric currents develop in regions of strong density gradients to balance the resulting plasma pressure gradients. These currents, usually known as diamagnetic currents decrease the magnetic pressure where the plasma pressure increases, and vice versa. In the low‐latitude ionosphere, equatorial plasma depletions (EPDs) are well known for their steep plasma density gradients and adverse effect on radio wave propagation. In this paper, we use continuous measurements of the magnetic field and electron density from the European Space Agency's Swarm constellation mission to assess the balance between plasma and magnetic pressure across large‐scale EPDs. The analysis is based on the magnetic fluctuations related to diamagnetic currents flowing at the edges of EPDs. This study shows that most of the EPDs detected by Swarm present a decrease of the plasma pressure relative to the ambient plasma. However, EPDs with high plasma pressure are also identified mainly in the vicinity of the South Atlantic magnetic anomaly. From the electron density measurements, we deduce that such an increase in plasma pressure within EPDs might be possible by temperatures inside the EPD as high as twice the temperature of the ambient plasma. Due to the distinct location of the high‐pressure EPDs, we suggest that a possible heating mechanism might be due to precipitation of particle from the radiation belts. This finding corresponds to the first observational evidence of plasma pressure enhancements in regions of depleted plasma density in the ionosphere.
Pitch Angle Scattering of Sub-MeV Relativistic Electrons by Electromagnetic Ion Cyclotron Waves
(2019)
Electromagnetic ion cyclotron (EMIC) waves have long been considered to be a significant loss mechanism for relativistic electrons. This has most often been attributed to resonant interactions with the highest amplitude waves. But recent observations have suggested that the dominant energy of electrons precipitated to the atmosphere may often be relatively low, less than 1 MeV, whereas the minimum resonant energy of the highest amplitude waves is often greater than 2 MeV. Here we use relativistic electron test particle simulations in the wavefields of a hybrid code simulation of EMIC waves in dipole geometry in order to show that significant pitch angle scattering can occur due to interaction with low-amplitude short-wavelength EMIC waves. In the case we examined, these waves are in the H band (at frequencies above the He+ gyrofrequency), even though the highest amplitude waves were in the He band frequency range (below the He+ gyrofrequency). We also present wave power distributions for 29 EMIC simulations in straight magnetic field line geometry that show that the high wave number portion of the spectrum is in every case mostly due to the H band waves. Though He band waves are often associated with relativistic electron precipitation, it is possible that the He band waves do not directly scatter the sub-megaelectron volts (sub-MeV) electrons, but that the presence of He band waves is associated with high plasma density which lowers the minimum resonant energy so that these electrons can more easily resonate with the H band waves.
In globally coupled ensembles of identical oscillators so-called chimera states can be observed. The chimera state is a symmetry-broken regime, where a subset of oscillators forms a cluster, a synchronized population, while the rest of the system remains a collection of nonsynchronized, scattered units. We describe here a blinking chimera regime in an ensemble of seven globally coupled rotators (Kuramoto oscillators with inertia). It is characterized by a death-birth process, where a long-term stable cluster of four oscillators suddenly dissolves and is very quickly reborn with a new reshuffled configuration. We identify three different kinds of rare blinking events and give a quantitative characterization by applying stability analysis to the long-lived chaotic state and to the short-lived regular regimes that arise when the cluster dissolves.
2D Ruddlesden-Popper perovskite (RPP) solar cells have excellent environmental stability. However, the power conversion efficiency (PCE) of RPP cells remains inferior to 3D perovskite-based cells. Herein, 2D (CH3(CH2)(3)NH3)(2)(CH3NH3)(n-1)PbnI3n+1 perovskite cells with different numbers of [PbI6](4-) sheets (n = 2-4) are analyzed. Photoluminescence quantum yield (PLQY) measurements show that nonradiative open-circuit voltage (V-OC) losses outweigh radiative losses in materials with n > 2. The n = 3 and n = 4 films exhibit a higher PLQY than the standard 3D methylammonium lead iodide perovskite although this is accompanied by increased interfacial recombination at the top perovskite/C-60 interface. This tradeoff results in a similar PLQY in all devices, including the n = 2 system where the perovskite bulk dominates the recombination properties of the cell. In most cases the quasi-Fermi level splitting matches the device V-OC within 20 meV, which indicates minimal recombination losses at the metal contacts. The results show that poor charge transport rather than exciton dissociation is the primary reason for the reduction in fill factor of the RPP devices. Optimized n = 4 RPP solar cells had PCEs of 13% with significant potential for further improvements.
Charge-density rearrangements after metal-to-ligand charge-transfer excitation in an iron photosensitizer are investigated by R. M Jay, A. Fohlisch et al. in their Communication (DOI: 10.1002/anie.201904761). By using time-resolved X-ray absorption spectroscopy, surprising covalency-effects are revealed that inhibit charge-separation at the intra-molecular level. Furthermore, the underlying mechanism is proposed to be generally in effect for all commonly used photosensitizers in light-harvesting applications, which challenges the common perception of electronic charge-transfer.
Context. Pulsar wind nebulae (PWNe) represent the most prominent population of Galactic very-high-energy gamma-ray sources and are thought to be an efficient source of leptonic cosmic rays. Vela X is a nearby middle-aged PWN, which shows bright X-ray and TeV gamma-ray emission towards an elongated structure called the cocoon. Aims. Since TeV emission is likely inverse-Compton emission of electrons, predominantly from interactions with the cosmic microwave background, while X-ray emission is synchrotron radiation of the same electrons, we aim to derive the properties of the relativistic particles and of magnetic fields with minimal modelling. Methods. We used data from the Suzaku XIS to derive the spectra from three compact regions in Vela X covering distances from 0.3 to 4 pc from the pulsar along the cocoon. We obtained gamma-ray spectra of the same regions from H.E.S.S. observations and fitted a radiative model to the multi-wavelength spectra. Results. The TeV electron spectra and magnetic field strengths are consistent within the uncertainties for the three regions, with energy densities of the order 10(-12) erg cm(-3). The data indicate the presence of a cutoff in the electron spectrum at energies of similar to 100 TeV and a magnetic field strength of similar to 6 mu G. Constraints on the presence of turbulent magnetic fields are weak. Conclusions. The pressure of TeV electrons and magnetic fields in the cocoon is dynamically negligible, requiring the presence of another dominant pressure component to balance the pulsar wind at the termination shock. Sub-TeV electrons cannot completely account for the missing pressure, which may be provided either by relativistic ions or from mixing of the ejecta with the pulsar wind. The electron spectra are consistent with expectations from transport scenarios dominated either by advection via the reverse shock or by diffusion, but for the latter the role of radiative losses near the termination shock needs to be further investigated in the light of the measured cutoff energies. Constraints on turbulent magnetic fields and the shape of the electron cutoff can be improved by spectral measurements in the energy range greater than or similar to 10 keV.
We demonstrate that femtosecond laser pulses allow triggering high-frequency standing spin-wave modes in nanoscale thin films of a bismuth-substituted yttrium iron garnet. By varying the strength of the external magnetic field, we prove that two distinct branches of the dispersion relation are excited for all the modes. This is reflected in particular at a very weak magnetic field (similar to 33 mT) by a spin dynamics with a frequency up to 15 GHz, which is 15 times higher than the one associated with the ferromagnetic resonance mode. We argue that this phenomenon is triggered by ultrafast changes of the magnetic anisotropy via laser excitation of incoherent and coherent phonons. These findings open exciting prospects for ultrafast photo magnonics.