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Strong light-matter coupling can re-arrange the exciton energies in organic semiconductors. Here, we exploit strong coupling by embedding a fullerene-free organic solar cell (OSC) photo-active layer into an optical microcavity, leading to the formation of polariton peaks and a red-shift of the optical gap. At the same time, the open-circuit voltage of the device remains unaffected. This leads to reduced photon energy losses for the low-energy polaritons and a steepening of the absorption edge. While strong coupling reduces the optical gap, the energy of the charge-transfer state is not affected for large driving force donor-acceptor systems. Interestingly, this implies that strong coupling can be exploited in OSCs to reduce the driving force for electron transfer, without chemical or microstructural modifications of the photoactive layer. Our work demonstrates that the processes determining voltage losses in OSCs can now be tuned, and reduced to unprecedented values, simply by manipulating the device architecture.
Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V-OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V-OC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V-OC of the device. Importantly, the V-OC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the V-OC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the V-OC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces.
Perovskite solar cells (PSCs) are one of the main research topics of the photovoltaic community; with efficiencies now reaching up to 24%, PSCs are on the way to catching up with classical inorganic solar cells. However, PSCs have not yet reached their full potential. In fact, their efficiency is still limited by nonradiative recombination, mainly via trap-states and by losses due to the poor transport properties of the commonly used transport layers (TLs). Indeed, state-of-the-art TLs (especially if organic) suffer from rather low mobilities, typically within 10(-5) and 10(-2) cm(-2) V-1 s(-1), when compared to the high mobilities, 1-10 cm(-2) V-1 s(-1), measured for perovskites. This work presents a comprehensive analysis of the effect of the mobility, thickness, and doping density of the transport layers based on combined experimental and modeling results of two sets of devices made of a solution-processed high-performing triple-cation (PCE approximate to 20%). The results are also cross-checked on vacuum-processed MAPbI(3) devices. From this analysis, general guidelines on how to optimize a TL are introduced and especially a new and simple formula to easily calculate the amount of doping necessary to counterbalance the low mobility of the TLs.
Context. On 27 April 2015, when comet 67P/Churyumov-Gerasimenko was at 1.76 au from the Sun and moving toward perihelion, the OSIRIS and VIRTIS-M instruments on board the Rosetta spacecraft simultaneously observed the evolving dust and gas coma during a complete rotation of the comet. Aims. We aim to characterize the spatial distribution of dust, H2O, and CO2 gas in the inner coma. To do this, we performed a quantitative analysis of the release of dust and gas and compared the observed H2O production rate with the rate we calculated using a thermophysical model. Methods. For this study we selected OSIRIS WAC images at 612 nm (dust) and VIRTIS-M image cubes at 612 nm, 2700 nm (H2O emission band), and 4200 nm (CO2 emission band). We measured the average signal in a circular annulus to study the spatial variation around the comet, and in a sector of the annulus to study temporal variation in the sunward direction with comet rotation, both at a fixed distance of 3.1 km from the comet center. Results. The spatial correlation between dust and water, both coming from the sunlit side of the comet, shows that water is the main driver of dust activity in this time period. The spatial distribution of CO2 is not correlated with water and dust. There is no strong temporal correlation between the dust brightness and water production rate as the comet rotates. The dust brightness shows a peak at 0 degrees subsolar longitude, which is not pronounced in the water production. At the same epoch, there is also a maximum in CO2 production. An excess of measured water production with respect to the value calculated using a simple thermophysical model is observed when the head lobe and regions of the southern hemisphere with strong seasonal variations are illuminated (subsolar longitude 270 degrees-50 degrees). A drastic decrease in dust production when the water production (both measured and from the model) displays a maximum occurs when typical northern consolidated regions are illuminated and the southern hemisphere regions with strong seasonal variations are instead in shadow (subsolar longitude 50 degrees-90 degrees). Possible explanations of these observations are presented and discussed.
On 2015 July 18, near perihelion at a heliocentric distance of 1.28 au, the Visible InfraRed Thermal Imaging Spectrometer (VIRTIS-M) on board the Rosetta spacecraft had the opportunity of observing dust activity in the inner coma with a view of the night side (shadowed side) of comet 67P/Churyumov-Gerasimenko. At the time of the measurements we present here, we observe a dust plume that originates on the far side of the nucleus. We are able to identify the approximate location of its source at the boundary between the Hapi and Anuket regions, and we find that it has been in darkness for some hours before the observation. Assuming that this time span is equal to the conductive time scale, we obtain a thermal inertia in the range 25-36 W K-1 m(-2) s(-1/2). These thermal inertia values can be used to verify with a 3D finite-element method (REM) numerical code whether the surface and subsurface temperatures agree with the values found in the literature. We explored three different configurations: (1) a layer of water ice mixed with dust beneath a dust mantle of 5 mm with thermal inertia of 36 J m(-2) K-1 S-0.5 ; (2) the same structure, but with thermal inertia of 100 J m(-2) K-1 S-0.5; (3) an ice-dust mixture that is directly exposed. Of these three configurations, the first seems to be the most reasonable, both for the low thermal inertia and for the agreement with the surface and subsurface temperatures that have been found for the comet 67P/Churyumov-Gerasimenko. The spectral properties of the plume show that the visible dust color ranged from 16 +/- 4.8%/100 nm to 13 +/- 2.6%/100 nm, indicating that this plume has no detectable color gradient. The morphology of the plume can be classified as a narrow jet that has an estimated total ejected mass of between 6 and 19 tons when we assume size distribution indices between -2.5 and -3.
Time-resolved crystallography reveals allosteric communication aligned with molecular breathing
(2019)
A comprehensive understanding of protein function demands correlating structure and dynamic changes. Using time-resolved serial synchrotron crystallography, we visualized half-of-the-sites reactivity and correlated molecular-breathing motions in the enzyme fluoroacetate dehalogenase. Eighteen time points from 30 milliseconds to 30 seconds cover four turnover cycles of the irreversible reaction. They reveal sequential substrate binding, covalent-intermediate formation, setup of a hydrolytic water molecule, and product release. Small structural changes of the protein mold and variations in the number and placement of water molecules accompany the various chemical steps of catalysis. Triggered by enzyme-ligand interactions, these repetitive changes in the protein framework’s dynamics and entropy constitute crucial components of the catalytic machinery.
We investigate spin-wave resonance modes and their damping in insulating thin films of bismuth-substituted yttrium iron garnet by performing femtosecond magneto-optical pump-probe experiments. For large magnetic fields in the range below the magnetization saturation, we find that the damping of high-order standing spin-wave (SSW) modes is about 40 times lower than that for the fundamental one. The observed phenomenon can be explained by considering different features of magnetic anisotropy and exchange fields that, respectively, define the precession frequency for fundamental and high-order SSWs. These results provide further insight into SSWs in iron garnets and may be exploited in many new photomagnonic devices.
We consider the first-passage problem for N identical independent particles that are initially released uniformly in a finite domain Ω and then diffuse toward a reactive area Γ, which can be part of the outer boundary of Ω or a reaction centre in the interior of Ω. For both cases of perfect and partial reactions, we obtain the explicit formulas for the first two moments of the fastest first-passage time (fFPT), i.e., the time when the first out of the N particles reacts with Γ. Moreover, we investigate the full probability density of the fFPT. We discuss a significant role of the initial condition in the scaling of the average fFPT with the particle number N, namely, a much stronger dependence (1/N and 1/N² for partially and perfectly reactive targets, respectively), in contrast to the well known inverse-logarithmic behaviour found when all particles are released from the same fixed point. We combine analytic solutions with scaling arguments and stochastic simulations to rationalise our results, which open new perspectives for studying the relevance of multiple searchers in various situations of molecular reactions, in particular, in living cells.
We present an analysis of two pulsating subdwarf B stars PHL 457 and EQ Psc observed during the K2 mission. The K2 light curves of both stars show variation consistent with irradiation of a cooler companion by the hot subdwarf. They also show higher frequency oscillations consistent with pulsation. Using new spectroscopic data, we measured the radial velocity, effective temperature, surface gravity, and helium abundance of both hot subdwarfs as a function of orbital phase. We confirm the previously published spectroscopic orbit of PHL 457, and present the first spectroscopic orbit of EQ Psc. The orbital periods are 0.313 and 0.801 d, respectively. For EQPsc, we find a strong correlation between T-eff and orbital phase, due to contribution of light from the irradiated companion. We calculated amplitude spectra, identified significant pulsation frequencies, and searched for multiplets and asymptotic period spacings. By means of multiplets and period spacing, we identified the degrees of several pulsation modes in each star. The g-mode multiplets indicate subsynchronous core rotation with periods of 4.6 d (PHL 457) and 9.4 d (EQ Psc). We made spectral energy disctribution (SED) fits of PHL 457 and EQ Psc using available broad-band photometry and Gaia data. While the SED of PHL 457 shows no evidence of a cool companion, the SED for EQPsc clearly shows an infrared (IR) access consistent with a secondary with a temperature of about 6800K and a radius of 0.23 R-circle dot. This is the first detection of an IR access in any sdB + dM binary.
“A chain is only as strong as its weakest link” says the proverb. But what about a collection of statistically identical chains: How long till all chains fail? The answer to this question is given by the max-min of a matrix whose (i,j)entry is the failure time of link j of chain i: take the minimum of each row, and then the maximum of the rows' minima. The corresponding min-max is obtained by taking the maximum of each column, and then the minimum of the columns' maxima. The min-max applies to the storage of critical data. Indeed, consider multiple backup copies of a set of critical data items, and consider the (i,j) matrix entry to be the time at which item j on copy i is lost; then, the min-max is the time at which the first critical data item is lost. In this paper we address random matrices whose entries are independent and identically distributed random variables. We establish Poisson-process limit laws for the row's minima and for the columns' maxima. Then, we further establish Gumbel limit laws for the max-min and for the min-max. The limit laws hold whenever the entries' distribution has a density, and yield highly applicable approximation tools and design tools for the max-min and min-max of large random matrices. A brief of the results presented herein is given in: Gumbel central limit theorem for max-min and min-max
The max-min and min-max of matrices arise prevalently in science and engineering. However, in many real-world situations the computation of the max-min and min-max is challenging as matrices are large and full information about their entries is lacking. Here we take a statistical-physics approach and establish limit laws—akin to the central limit theorem—for the max-min and min-max of large random matrices. The limit laws intertwine random-matrix theory and extreme-value theory, couple the matrix dimensions geometrically, and assert that Gumbel statistics emerge irrespective of the matrix entries' distribution. Due to their generality and universality, as well as their practicality, these results are expected to have a host of applications in the physical sciences and beyond.
High-density polyethylene becomes optically transparent during tensile drawing when previously saturated with diesel fuel. This unusual phenomenon is investigated as it might allow conclusions with respect to the material behavior. Microscopy, differential scanning calorimetry, density measurements are applied together with two scanning X-ray scattering techniques: wide angle X-ray scattering (WAXS) and X-ray refraction, able to extract the spatially resolved crystal orientation and internal surface, respectively. The sorbed diesel softens the material and significantly alters the yielding characteristics. Although the crystallinity among stretched regions is similar, a virgin reference sample exhibits strain whitening during stretching, while the diesel-saturated sample becomes transparent. The WAXS results reveal a pronounced fiber texture in the tensile direction in the stretched region and an isotropic orientation in the unstretched region. This texture implies the formation of fibrils in the stretched region, while spherulites remain intact in the unstretched parts of the specimens. X-ray refraction reveals a preferred orientation of internal surfaces along the tensile direction in the stretched region of virgin samples, while the sample stretched in the diesel-saturated state shows no internal surfaces at all. Besides from stretching saturated samples, optical transparency is also obtained from sorbing samples in diesel after stretching.
We numerically and analytically analyze transitions between different synchronous states in a network of globally coupled phase oscillators with attractive and repulsive interactions. The elements within the attractive or repulsive group are identical, but natural frequencies of the groups differ. In addition to a synchronous two-cluster state, the system exhibits a solitary state, when a single oscillator leaves the cluster of repulsive elements, as well as partially synchronous quasiperiodic dynamics. We demonstrate how the transitions between these states occur when the repulsion starts to prevail over attraction.
Aims. In this study, we analyzed a filament system, which expanded between moving magnetic features (MMFs) of a decaying sunspot and opposite flux outside of the active region from the nearby quiet-Sun network. This configuration deviated from a classical arch filament system (AFS), which typically connects two pores in an emerging flux region. Thus, we called this system an extended AFS. We contrasted classical and extended AFSs with an emphasis on the complex magnetic structure of the latter. Furthermore, we examined the physical properties of the extended AFS and described its dynamics and connectivity. Methods. The extended AFS was observed with two instruments at the Dunn Solar Telescope (DST). The Rapid Oscillations in the Solar Atmosphere (ROSA) imager provided images in three different wavelength regions, which covered the dynamics of the extended AFS at different atmospheric heights. The Interferometric Bidimensional Spectropolarimeter (IBIS) provided spectroscopic Ha data and spectropolarimetric data that was obtained in the near-infrared (NIR) Call lambda 8542 angstrom line. We derived the corresponding line-of-sight (LOS) velocities and used He II lambda 304 angstrom extreme ultraviolet (EUV) images of the Atmospheric Imaging Assembly (AIA) and LOS magnetograms of the Helioseismic and Magnetic Imager (HMI) on board the Solar Dynamics Observatory (SDO) as context data. Results. The NIR Call Stokes-V maps are not suitable to definitively define a clear polarity inversion line and to classify this chromospheric structure. Nevertheless, this unusual AFS connects the MMFs of a decaying sunspot with the network field. At the southern footpoint, we measured that the flux decreases over time. We find strong downflow velocities at the footpoints of the extended AFS, which increase in a time period of 30 min. The velocities are asymmetric at both footpoints with higher velocities at the southern footpoint. An EUV brigthening appears in one of the arch filaments, which migrates from the northern footpoint toward the southern one. This activation likely influences the increasing redshift at the southern footpoint. Conclusions. The extended AFS exhibits a similar morphology as classical AFSs, for example, threaded filaments of comparable length and width. Major differences concern the connection from MMFs around the sunspot with the flux of the neighboring quietSun network, converging footpoint motions, and longer lifetimes of individual arch filaments of about one hour, while the extended AFS is still very dynamic.
The in-depth understanding of charge carrier photogeneration and recombination mechanisms in organic solar cells is still an ongoing effort. In donor:acceptor (bulk) heterojunction organic solar cells, charge photogeneration and recombination are inter-related via the kinetics of charge transfer states-being singlet or triplet states. Although high-charge-photogeneration quantum yields are achieved in many donor:acceptor systems, only very few systems show significantly reduced bimolecular recombination relative to the rate of free carrier encounters, in low-mobility systems. This is a serious limitation for the industrialization of organic solar cells, in particular when aiming at thick active layers. Herein, a meta-analysis of the device performance of numerous bulk heterojunction organic solar cells is presented for which field-dependent photogeneration, charge carrier mobility, and fill factor are determined. Herein, a "spin-related factor" that is dependent on the ratio of back electron transfer of the triplet charge transfer (CT) states to the decay rate of the singlet CT states is introduced. It is shown that this factor links the recombination reduction factor to charge-generation efficiency. As a consequence, it is only in the systems with very efficient charge generation and very fast CT dissociation that free carrier recombination is strongly suppressed, regardless of the spin-related factor.
Supercritical Kuramoto oscillators with distributed frequencies can be separated into two disjoint groups: an ordered one locked to the mean field, and a disordered one consisting of effectively decoupled oscillators-at least so in the thermodynamic limit. In finite ensembles, in contrast, such clear separation fails: The mean field fluctuates due to finite-size effects and thereby induces order in the disordered group. This publication demonstrates this effect, similar to noise-induced synchronization, in a purely deterministic system. We start by modeling the situation as a stationary mean field with additional white noise acting on a pair of unlocked Kuramoto oscillators. An analytical expression shows that the cross-correlation between the two increases with decreasing ratio of natural frequency difference and noise intensity. In a deterministic finite Kuramoto model, the strength of the mean-field fluctuations is inextricably linked to the typical natural frequency difference. Therefore, we let a fluctuating mean field, generated by a finite ensemble of active oscillators, act on pairs of passive oscillators with a microscopic natural frequency difference between which we then measure the cross-correlation, at both super- and subcritical coupling.
The purity of the analysed samples (e.g. quartz) with respect to chemical composition and radionuclide contamination is essential for geomorphologic applications using so-called terrestrial cosmogenic nuclides (TCNs). To guarantee this, numerous cleaning and dissolution procedures have been developed. At the DREsden Accelerator Mass Spectrometry (DREAMS) facility, we also work on enhancing the chemical quartz-enrichment methodology from bulk rock and dissolution of quartz. Repeated exposure of the bulk material to acid mixtures (HCl/H2SiF6) at room temperature for cleaning and its monitoring by optical microscopy works for most quartz-rich samples. The quartz dissolution in HF under rather mild conditions (at room temperature on a shaker-table) has the advantage to leave difficult-to-dissolve minerals (e.g., tourmaline, zircon, rutile, sillimanite, kyanite, chromite, corundum), not separated by other physical methods before, as residue. Our comparison with a high-temperature dissolution method (in a microwave) indicates an additional amount of interfering elements, such as in average about 3 mg of Ti, more than 7 mg of Al, and about 22 mu g of Be (for 50 g SiO2), is added to the sample, hence showing the superiority of our mild method. This way, we reduce problems for chemistry and AMS, but also ensure better comparability to production rates of cleaner stoichiometric quartz from calibration sites.
Simulations of the inner magnetospheric energetic electrons using the IMPTAM-VERB coupled model
(2019)
In this study, we present initial results of the coupling between the Inner Magnetospheric Particle Transport and Acceleration Model (IMPTAM) and the Versatile Electron Radiation Belt (VERB-3D) code. IMPTAM traces electrons of 10-100 keV energies from the plasma sheet (L = 9 Re) to inner L-shell regions. The flux evolution modeled by IMPTAM is used at the low energy and outer L* computational boundaries of the VERB code (assuming a dipole approximation) to perform radiation belt simulations of energetic electrons. The model was tested on the March 17th, 2013 storm, for a six-day period. Four different simulations were performed and their results compared to satellites observations from Van Allen probes and GOES. The coupled IMPTAM-VERB model reproduces evolution and storm-time features of electron fluxes throughout the studied storm in agreement with the satellite data (within similar to 0.5 orders of magnitude). Including dynamics of the low energy population at L* = 6.6 increases fluxes closer to the heart of the belt and has a strong impact in the VERB simulations at all energies. However, inclusion of magnetopause losses leads to drastic flux decreases even below L* = 3. The dynamics of low energy electrons (max. 10s of keV) do not affect electron fluxes at energies >= 900 keV. Since the IMPTAM-VERB coupled model is only driven by solar wind parameters and the Dst and Kp indexes, it is suitable as a forecasting tool. In this study, we demonstrate that the estimation of electron dynamics with satellite-data-independent models is possible and very accurate.
Holocene glacial chronostratigraphies in glaciated valleys spread throughout the Himalayan-Tibetan orogen, including the Himalaya, Tibet, Pamir, and Tian Shan, are developed using a landsystems approach, detailed geomorphic mapping, and new and published Be-10 surface exposure dating. New studies in the Kulti valley of Lahul and the Parkachik valley of the Nun Kun massif of the Himalaya of northern India define three glacier advances at similar to 14.7, 12.2, 0.5 ka, in addition to one historically dated late 19th Century advance in the Kulti valley, and one Late Holocene advance at similar to 0.2 ka in the Parkachik valley. Three major climatic groups (subdivided into five climatic zones) are defined across the orogen using Cluster Analysis (CA) and Principal Component Analysis (PCA) to identify glaciated regions with comparable climatic characteristics to evaluate the timing, and extent of Holocene glacier advances across these regions. Our regional analyses across the Himalayan-Tibetan orogen suggest at least one Lateglacial (similar to 15.3-11.8 ka) and five Himalayan-Tibetan Holocene glacial stages (HTHS) at similar to 11.5-9.5, similar to 8.8-7.7, similar to 7.0-3.2, similar to 2.3-1.0, and <1 ka. The extent (amplitude) of glacier advances in 77 glaciated valleys is reconstructed and defined using equilibrium-line altitudes (ELAs). Modern glacier hypsometries are also assessed to help explain the intra-regional variations in glacier amplitudes during each regional glacier advance. A linear inverse glacier flow model is used to decipher the net changes in temperature (Delta T) between periods of reconstructed regional glacier advances in 66 glaciated valleys across different climatic regions throughout the orogen. The Be-10, ELAs, and Delta T data suggest enhanced monsoonal and increased precipitation during the Early Holocene, followed by relative cooling and increased aridity during the Mid- and Late Holocene that influenced glaciation. The sublimation-dominated cold-based glaciers in the northern regions of Himalayan-Tibetan orogen are more affected during these shifts in climate than the temperate glaciers in the south. (C) 2019 Elsevier Ltd. All rights reserved.