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The oceans and atmosphere interact via a multiplicity of feedback mechanisms, shaping to a large extent the global climate and its variability. To deepen our knowledge of the global climate system, characterizing and investigating this interdependence is an important task of contemporary research. However, our present understanding of the underlying large-scale processes is greatly limited due to the manifold interactions between essential climatic variables at different temporal scales. To address this problem, we here propose to extend the application of complex network techniques to capture the interdependence between global fields of sea-surface temperature (SST) and precipitation (P) at multiple temporal scales. For this purpose, we combine time-scale decomposition by means of a discrete wavelet transform with the concept of coupled climate network analysis. Our results demonstrate the potential of the proposed approach to unravel the scale-specific interdependences between atmosphere and ocean and, thus, shed light on the emerging multiscale processes inherent to the climate system, which traditionally remain undiscovered when investigating the system only at the native resolution of existing climate data sets. Moreover, we show how the relevant spatial interdependence structures between SST and P evolve across time-scales. Most notably, the strongest mutual correlations between SST and P at annual scale (8-16 months) concentrate mainly over the Pacific Ocean, while the corresponding spatial patterns progressively disappear when moving toward longer time-scales. Published under license by AIP Publishing.
We investigate the predictive power of recurrent neural networks for oscillatory systems not only on the attractor but in its vicinity as well. For this, we consider systems perturbed by an external force. This allows us to not merely predict the time evolution of the system but also study its dynamical properties, such as bifurcations, dynamical response curves, characteristic exponents, etc. It is shown that they can be effectively estimated even in some regions of the state space where no input data were given. We consider several different oscillatory examples, including self-sustained, excitatory, time-delay, and chaotic systems. Furthermore, with a statistical analysis, we assess the amount of training data required for effective inference for two common recurrent neural network cells, the long short-term memory and the gated recurrent unit. Published under license by AIP Publishing.
In this study, rapid loss of relativistic radiation belt electrons at low L* values (2.4-3.2) during a strong geomagnetic storm on 22 June 2015 is investigated along with five possible loss mechanisms. Both the particle and wave data are obtained from the Van Allen Probes. Duskside H+ band electromagnetic ion cyclotron (EMIC) waves were observed during a rapid decrease of relativistic electrons with energy above 5.2 MeV occurring outside the plasma sphere during extreme magnetopause compression. Lower He+ composition and enriched O+ composition are found compared to typical values assumed in other studies of cyclotron resonant scattering of relativistic electrons by EMIC waves. Quantitative analysis demonstrates that even with the existence of He+ band EMIC waves, it is the H+ band EMIC waves that are likely to cause the depletion at small pitch angles and strong gradients in pitch angle distributions of relativistic electrons with energy above 5.2 MeV at low L values for this event. Very low frequency wave activity at other magnetic local time can be favorable for the loss of relativistic electrons at higher pitch angles. An illustrative calculation that combines the nominal pitch angle scattering rate due to whistler mode chorus at high pitch angles with the H+ band EMIC wave loss rate at low pitch angles produces loss on time scale observed at L = 2.4-3.2. At high L values and lower energies, radial loss to the magnetopause is a viable explanation.
The functionality of organic semiconductor devices crucially depends on molecular energies, namely the ionisation energy and the electron affinity. Ionisation energy and electron affinity values of thin films are, however, sensitive to film morphology and composition, making their prediction challenging. In a combined experimental and simulation study on zinc-phthalocyanine and its fluorinated derivatives, we show that changes in ionisation energy as a function of molecular orientation in neat films or mixing ratio in blends are proportional to the molecular quadrupole component along the p-p-stacking direction. We apply these findings to organic solar cells and demonstrate how the electrostatic interactions can be tuned to optimise the energy of the charge-transfer state at the donor-acceptor interface and the dissociation barrier for free charge carrier generation. The confirmation of the correlation between interfacial energies and quadrupole moments for other materials indicates its relevance for small molecules and polymers.
An understanding of the factors limiting the open-circuit voltage (V-oc) and related photon energy loss mechanisms is critical to increase the power conversion efficiency (PCE) of small-molecule organic solar cells (OSCs), especially those with near-infrared (NIR) absorbers. In this work, two NIR boron dipyrromethene (BODIPY) molecules are characterized for application in planar (PHJ) and bulk (BHJ) heterojunction OSCs. When two H atoms are substituted by F atoms on the peripheral phenyl rings of the molecules, the molecular aggregation type in the thin film changes from the H-type to J-type. For PHJ devices, the nonradiative voltage loss of 0.35 V in the J-aggregated BODIPY is lower than that of 0.49 V in the H-aggregated device. In BHJ devices with a nonradiative voltage loss of 0.35 V, a PCE of 5.5% is achieved with an external quantum efficiency (EQE) maximum of 68% at 700 nm.
The optimized design of multilayer-coated blazed gratings (MLBG) for high-flux tender X-ray monochromators was systematically studied by numerical simulations. The resulting correlation between the multilayer d-spacing and grating blaze angle significantly deviated from the one predicted by conventional equations. Three high line density gratings with different blaze angles were fabricated and coated by the same Cr/C multilayer. The MLBG with an optimal blaze angle of 1.0 degrees showed a record efficiency reaching 60% at 3.1 keV and 4.1 keV. The measured efficiencies of all three gratings were consistent with calculated results proving the validity of the numerical simulation and indicating a more rigorous way to design the optimal MLBG structure. Published by The Optical Society under the terms of the Creative Commons Attribution 4.0 License.
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.