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Charge carrier recombination in organic disordered semiconductors is strongly influenced by the thermalization of charge carriers in the density of states (DOS). Measurements of recombination dynamics, conducted under transient or steady-state conditions, can easily be misinterpreted when a detailed understanding of the interplay of thermalization and recombination is missing. To enable adequate measurement analysis, we solve the multiple-trapping problem for recombining charge carriers and analyze it in the transient and steady excitation paradigm for different DOS distributions. We show that recombination rates measured after pulsed excitation are inherently time dependent since recombination gradually slows down as carriers relax in the DOS. When measuring the recombination order after pulsed excitation, this leads to an apparent high-order recombination at short times. As times goes on, the recombination order approaches an asymptotic value. For the Gaussian and the exponential DOS distributions, this asymptotic value equals the recombination order of the equilibrated system under steady excitation. For a more general DOS distribution, the recombination order can also depend on the carrier density, under both transient and steady-state conditions. We conclude that transient experiments can provide rich information about recombination in and out of equilibrium and the underlying DOS occupation provided that consistent modeling of the system is performed.
In this Letter, we study the role of the donor:acceptor interface nanostructure upon charge separation and recombination in organic photovoltaic devices and blend films, using mixtures of PBTTT and two different fullerene derivatives (PC70BM and ICTA) as models for intercalated and nonintercalated morphologies, respectively. Thermodynamic simulations show that while the completely intercalated system exhibits a large free-energy barrier for charge separation, this barrier is significantly lower in the nonintercalated system and almost vanishes when energetic disorder is included in the model. Despite these differences, both femtosecond-resolved transient absorption spectroscopy (TAS) and time-delayed collection field (TDCF) exhibit extensive first-order losses in both systems, suggesting that geminate pairs are the primary product of photoexcitation. In contrast, the system that comprises a combination of fully intercalated polymer:fullerene areas and fullerene-aggregated domains (1:4 PBTTT:PC70BM) is the only one that shows slow, second-order recombination of free charges, resulting in devices with an overall higher short-circuit current and fill factor. This study therefore provides a novel consideration of the role of the interfacial nanostructure and the nature of bound charges and their impact upon charge generation and recombination.
High photon energy losses limit the open-circuit voltage (V-OC) and power conversion efficiency of organic solar cells (OSCs). In this work, an optimization route is presented which increases the V-OC by reducing the interfacial area between donor (D) and acceptor (A). This optimization route concerns a cascade device architecture in which the introduction of discontinuous interlayers between alpha-sexithiophene (alpha-6T) (D) and chloroboron subnaphthalocyanine (SubNc) (A) increases the V-OC of an alpha-6T/SubNc/SubPc fullerene-free cascade OSC from 0.98 V to 1.16 V. This increase of 0.18 V is attributed solely to the suppression of nonradiative recombination at the D-A interface. By accurately measuring the optical gap (E-opt) and the energy of the charge-transfer state (E-CT) of the studied OSC, a detailed analysis of the overall voltage losses is performed. E-opt - qV(OC) losses of 0.58 eV, which are among the lowest observed for OSCs, are obtained. Most importantly, for the V-OC-optimized devices, the low-energy (700 nm) external quantum efficiency (EQE) peak remains high at 79%, despite a minimal driving force for charge separation of less than 10 meV. This work shows that low-voltage losses can be combined with a high EQE in organic photovoltaic devices.
Charge carrier recombination in organic disordered semiconductors is strongly influenced by the thermalization of charge carriers in the density of states (DOS). Measurements of recombination dynamics, conducted under transient or steady-state conditions, can easily be misinterpreted when a detailed understanding of the interplay of thermalization and recombination is missing. To enable adequate measurement analysis, we solve the multiple-trapping problem for recombining charge carriers and analyze it in the transient and steady excitation paradigm for different DOS distributions. We show that recombination rates measured after pulsed excitation are inherently time dependent since recombination gradually slows down as carriers relax in the DOS. When measuring the recombination order after pulsed excitation, this leads to an apparent high-order recombination at short times. As times goes on, the recombination order approaches an asymptotic value. For the Gaussian and the exponential DOS distributions, this asymptotic value equals the recombination order of the equilibrated system under steady excitation. For a more general DOS distribution, the recombination order can also depend on the carrier density, under both transient and steady-state conditions. We conclude that transient experiments can provide rich information about recombination in and out of equilibrium and the underlying DOS occupation provided that consistent modeling of the system is performed.
We present a setup combining a liquid flatjet sample delivery and a MHz laser system for time-resolved soft X-ray absorption measurements of liquid samples at the high brilliance undulator beamline UE52-SGM at Bessy II yielding unprecedented statistics in this spectral range. We demonstrate that the efficient detection of transient absorption changes in transmission mode enables the identification of photoexcited species in dilute samples. With iron(II)-trisbipyridine in aqueous solution as a benchmark system, we present absorption measurements at various edges in the soft X-ray regime. In combination with the wavelength tunability of the laser system, the set-up opens up opportunities to study the photochemistry of many systems at low concentrations, relevant to materials sciences, chemistry, and biology. (C) 2017 Author(s).
Simultaneous dynamic characterization of charge and structural motion during ferroelectric switching
(2017)
Monitoring structural changes in ferroelectric thin films during electric field induced polarization switching is important for a full microscopic understanding of the coupled motion of charges, atoms, and domainwalls in ferroelectric nanostructures. We combine standard ferroelectric test sequences of switching and nonswitching electrical pulses with time-resolved x-ray diffraction to investigate the structural response of a nanoscale Pb(Zr0.2Ti0.8)O-3 ferroelectric oxide capacitor upon charging, discharging, and polarization reversal. We observe that a nonlinear piezoelectric response of the ferroelectric layer develops on a much longer time scale than the RC time constant of the device. The complex atomic motion during the ferroelectric polarization reversal starts with a contraction of the lattice, whereas the expansive piezoelectric response sets in after considerable charge flow due to the applied voltage pulses on the electrodes of the capacitor. Our simultaneous measurements on a working device elucidate and visualize the complex interplay of charge flow and structural motion and challenges theoretical modeling.
Despite the ongoing progress in nanotechnology and its applications, the development of strategies for connecting nano-scale systems to micro-or macroscale elements is hampered by the lack of structural components that have both, nano-and macroscale dimensions. The production of nano-scale wires with macroscale length is one of the most interesting challenges here. There are a lot of strategies to fabricate long nanoscopic stripes made of metals, polymers or ceramics but none is suitable for mass production of ordered and dense arrangements of wires at large numbers. In this paper, we report on a technique for producing arrays of ordered, flexible and free-standing polymer nano-wires filled with different types of nano-particles. The process utilizes the strong response of photosensitive polymer brushes to irradiation with UV-interference patterns, resulting in a substantial mass redistribution of the polymer material along with local rupturing of polymer chains. The chains can wind up in wires of nano-scale thickness and a length of up to several centimeters. When dispersing nano-particles within the film, the final arrangement is similar to a core-shell geometry with mainly nano-particles found in the core region and the polymer forming a dielectric jacket.
Despite the ongoing progress in nanotechnology and its applications, the development of strategies for connecting nano-scale systems to micro- or macroscale elements is hampered by the lack of structural components that have both, nano- and macroscale dimensions. The production of nano-scale wires with macroscale length is one of the most interesting challenges here. There are a lot of strategies to fabricate long nanoscopic stripes made of metals, polymers or ceramics but none is suitable for mass production of ordered and dense arrangements of wires at large numbers. In this paper, we report on a technique for producing arrays of ordered, flexible and free-standing polymer nano-wires filled with different types of nano-particles. The process utilizes the strong response of photosensitive polymer brushes to irradiation with UV-interference patterns, resulting in a substantial mass redistribution of the polymer material along with local rupturing of polymer chains. The chains can wind up in wires of nano-scale thickness and a length of up to several centimeters. When dispersing nano-particles within the film, the final arrangement is similar to a core-shell geometry with mainly nano-particles found in the core region and the polymer forming a dielectric jacket.
We investigate the heat transport through a rare earth multilayer system composed of yttrium (Y), dysprosium (Dy), and niobium (Nb) by ultrafast x-ray diffraction. This is an example of a complex heat flow problem on the nanoscale, where several different quasiparticles carry the heat and conserve a nonequilibrium for more than 10 ns. The Bragg peak positions of each layer represent layer-specific thermometers that measure the energy flow through the sample after excitation of the Y top layer with fs-laser pulses. In an experiment-based analytic solution to the nonequilibrium heat transport problem, we derive the individual contributions of the spins and the coupled electron-lattice system to the heat conduction. The full characterization of the spatiotemporal energy flow at different starting temperatures reveals that the spin excitations of antiferromagnetic Dy speed up the heat transport into the Dy layer at low temperatures, whereas the heat transport through this layer and further into the Y and Nb layers underneath is slowed down. The experimental findings are compared to the solution of the heat equation using macroscopic temperature-dependent material parameters without separation of spin and phonon contributions to the heat. We explain why the simulated energy density matches our experiment-based derivation of the heat transport, although the simulated thermoelastic strain in this simulation is not even in qualitative agreement.
Measurement of the EBL spectral energy distribution using the VHE gamma-ray spectra of HESS blazars
(2017)
Very high-energy gamma rays (VHE, E greater than or similar to 100 GeV) propagating over cosmological distances can interact with the low-energy photons of the extragalactic background light (EBL) and produce electron-positron pairs. The transparency of the Universe to VHE gamma rays is then directly related to the spectral energy distribution (SED) of the EBL. The observation of features in the VHE energy spectra of extragalactic sources allows the EBL to be measured, which otherwise is very difficult. An EBL model-independent measurement of the EBL SED with the H.E.S.S. array of Cherenkov telescopes is presented. It was obtained by extracting the EBL absorption signal from the reanalysis of high-quality spectra of blazars. From H.E.S.S. data alone the EBL signature is detected at a significance of 9.5 sigma, and the intensity of the EBL obtained in different spectral bands is presented together with the associated gamma-ray horizon.
We search for high-energy gamma-ray emission from the binary neutron star merger GW170817 with the H.E.S.S. Imaging Air Cherenkov Telescopes. The observations presented here have been obtained starting only 5.3 hr after GW170817. The H.E.S.S. target selection identified regions of high probability to find a counterpart of the gravitational-wave event. The first of these regions contained the counterpart SSS17a that has been identified in the optical range several hours after our observations. We can therefore present the first data obtained by a ground-based pointing instrument on this object. A subsequent monitoring campaign with the H.E.S.S. telescopes extended over several days, covering timescales from 0.22 to 5.2 days and energy ranges between 270 GeV to 8.55 TeV. No significant gamma-ray emission has been found. The derived upper limits on the very-high-energy gamma-ray flux for the first time constrain non-thermal, high-energy emission following the merger of a confirmed binary neutron star system.
We study triggering processes in triaxial compression experiments under a constant displacement rate on sandstone and granite samples using spatially located acoustic emission events and their focal mechanisms. We present strong evidence that event-event triggering plays an important role in the presence of large-scale or macrocopic imperfections, while such triggering is basically absent if no significant imperfections are present. In the former case, we recover all established empirical relations of aftershock seismicity including the Gutenberg-Richter relation, a modified version of the Omori-Utsu relation and the productivity relation-despite the fact that the activity is dominated by compaction-type events and triggering cascades have a swarmlike topology. For the Gutenberg-Richter relations, we find that the b value is smaller for triggered events compared to background events. Moreover, we show that triggered acoustic emission events have a focal mechanism much more similar to their associated trigger than expected by chance.
Despite the ongoing progress in nanotechnology and its applications, the development of strategies for connecting nano-scale systems to micro- or macroscale elements is hampered by the lack of structural components that have both, nano- and macroscale dimensions. The production of nano-scale wires with macroscale length is one of the most interesting challenges here. There are a lot of strategies to fabricate long nanoscopic stripes made of metals, polymers or ceramics but none is suitable for mass production of ordered and dense arrangements of wires at large numbers. In this paper, we report on a technique for producing arrays of ordered, flexible and free-standing polymer nano-wires filled with different types of nano-particles. The process utilizes the strong response of photosensitive polymer brushes to irradiation with UV-interference patterns, resulting in a substantial mass redistribution of the polymer material along with local rupturing of polymer chains. The chains can wind up in wires of nano-scale thickness and a length of up to several centimeters. When dispersing nano-particles within the film, the final arrangement is similar to a core-shell geometry with mainly nano-particles found in the core region and the polymer forming a dielectric jacket.
The significance of biogenic silicon (BSi) pools as a key factor for the control of Si fluxes from terrestrial to aquatic ecosystems has been recognized for decades. However, while most research has been focused on phytogenic Si pools, knowledge of other BSi pools is still limited. We hypothesized that different BSi pools influence short-term changes in the water-soluble Si fraction in soils to different extents. To test our hypothesis we took plant (Calamagrostis epigejos, Phragmites australis) and soil samples in an artificial catchment in a post-mining landscape in the state of Brandenburg, Germany. We quantified phytogenic (phytoliths), protistic (diatom frustules and testate amoeba shells) and zoogenic (sponge spicules) Si pools as well as Tironextractable and water-soluble Si fractions in soils at the beginning (t(0)) and after 10 years (t(10)) of ecosystem development. As expected the results of Tiron extraction showed that there are no consistent changes in the amorphous Si pool at Chicken Creek (Huhnerwasser) as early as after 10 years. In contrast to t(0) we found increased water-soluble Si and BSi pools at t(10); thus we concluded that BSi pools are the main driver of short-term changes in water-soluble Si. However, because total BSi represents only small proportions of water-soluble Si at t(0) (< 2 %) and t(10) (2.8-4.3 %) we further concluded that smaller (< 5 mu m) and/or fragile phytogenic Si structures have the biggest impact on short-term changes in water-soluble Si. In this context, extracted phytoliths (> 5 mu m) only amounted to about 16% of total Si con-tents of plant materials of C. epigejos and P. australis at t(10); thus about 84% of small-scale and/or fragile phytogenic Si is not quantified by the used phytolith extraction method. Analyses of small-scale and fragile phytogenic Si structures are urgently needed in future work as they seem to represent the biggest and most reactive Si pool in soils. Thus they are the most important drivers of Si cycling in terrestrial biogeosystems.
Aims. We study small-scale brightenings in Ca II 8542 angstrom line-core images to determine their nature and effect on localized heating and mass transfer in active regions. Methods. High-resolution two-dimensional spectroscopic observations of a solar active region in the near-infrared Ca II 8542 angstrom line were acquired with the GREGOR Fabry-Perot Interferometer attached to the 1.5-m GREGOR telescope. Inversions of the spectra were carried out using the NICOLE code to infer temperatures and line-of-sight (LOS) velocities. Response functions of the Ca II line were computed for temperature and LOS velocity variations. Filtergrams of the Atmospheric Imaging Assembly (AIA) and magnetograms of the Helioseismic and Magnetic Imager (HMI) were coaligned to match the ground-based observations and to follow the Ca II brightenings along all available layers of the atmosphere. Results. We identified three brightenings of sizes up to 2 ' x 2 ' that appeared in the Ca II 8542 angstrom line-core images. Their lifetimes were at least 1.5 min. We found evidence that the brightenings belonged to the footpoints of a microflare (MF). The properties of the observed brightenings disqualified the scenarios of Ellerman bombs or Interface Region Imaging Spectrograph (IRIS) bombs. However, this MF shared some common properties with flaring active-region fibrils or flaring arch filaments (FAFs): (1) FAFs and MFs are both apparent in chromospheric and coronal layers according to the AIA channels; and (2) both show flaring arches with lifetimes of about 3.0-3.5 min and lengths of similar to 20 ' next to the brightenings. The inversions revealed heating by 600 K at the footpoint location in the ambient chromosphere during the impulsive phase. Connecting the footpoints, a dark filamentary structure appeared in the Ca II line-core images. Before the start of the MF, the spectra of this structure already indicated average blueshifts, meaning upward motions of the plasma along the LOS. During the impulsive phase, these velocities increased up to -2.2 km s(-1). The structure did not disappear during the observations. Downflows dominated at the footpoints. However, in the upper photosphere, slight upflows occurred during the impulsive phase. Hence, bidirectional flows are present in the footpoints of the MF.