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Perovskite solar cells now compete with their inorganic counterparts in terms of power conversion efficiency, not least because of their small open-circuit voltage (V-OC) losses. A key to surpass traditional thin-film solar cells is the fill factor (FF). Therefore, more insights into the physical mechanisms that define the bias dependence of the photocurrent are urgently required. In this work, we studied charge extraction and recombination in efficient triple cation perovskite solar cells with undoped organic electron/hole transport layers (ETL/HTL). Using integral time of flight we identify the transit time through the HTL as the key figure of merit for maximizing the fill factor (FF) and efficiency. Complementarily, intensity dependent photocurrent and V-OC measurements elucidate the role of the HTL on the bias dependence of non-radiative and transport-related loss channels. We show that charge transport losses can be completely avoided under certain conditions, yielding devices with FFs of up to 84%. Optimized cells exhibit power conversion efficiencies of above 20% for 6 mm(2) sized pixels and 18.9% for a device area of 1 cm(2). These are record efficiencies for hybrid perovskite devices with dopant-free transport layers, highlighting the potential of this device technology to avoid charge-transport limitations and to approach the Shockley-Queisser limit.
Organic solar cells demonstrate external quantum efficiencies and fill factors approaching those of conventional photovoltaic technologies. However, as compared with the optical gap of the absorber materials, their open-circuit voltage is much lower, largely due to the presence of significant non-radiative recombination. Here, we study a large data set of published and new material combinations and find that non-radiative voltage losses decrease with increasing charge-transfer-state energies. This observation is explained by considering non-radiative charge-transfer-state decay as electron transfer in the Marcus inverted regime, being facilitated by a common skeletal molecular vibrational mode. Our results suggest an intrinsic link between non-radiative voltage losses and electron-vibration coupling, indicating that these losses are unavoidable. Accordingly, the theoretical upper limit for the power conversion efficiency of single-junction organic solar cells would be reduced to about 25.5% and the optimal optical gap increases to (1.45-1.65) eV, that is, (0.2-0.3) eV higher than for technologies with minimized non-radiative voltage losses.
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.
Reduced Interface-Mediated Recombination for High Open-Circuit Voltages in CH3NH3PbI3 Solar Cells
(2017)
Perovskite solar cells with all-organic transport layers exhibit efficiencies rivaling their counterparts that employ inorganic transport layers, while avoiding high-temperature processing. Herein, it is investigated how the choice of the fullerene derivative employed in the electron-transporting layer of inverted perovskite cells affects the open-circuit voltage (V-OC). It is shown that nonradiative recombination mediated by the electron-transporting layer is the limiting factor for the V-OC in the cells. By inserting an ultrathin layer of an insulating polymer between the active CH3NH3PbI3 perovskite and the fullerene, an external radiative efficiency of up to 0.3%, a V-OC as high as 1.16 V, and a power conversion efficiency of 19.4% are realized. The results show that the reduction of nonradiative recombination due to charge-blocking at the perovskite/organic interface is more important than proper level alignment in the search for ideal selective contacts toward high V-OC and efficiency.
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.
Electron flux in the Earth’s outer radiation belt is highly variable due to a delicate balance between competing acceleration and loss processes. It has been long recognized that Electromagnetic Ion Cyclotron (EMIC) waves may play a crucial role in the loss of radiation belt electrons. Previous theoretical studies proposed that EMIC waves may account for the loss of the relativistic electron population. However, recent observations showed that while EMIC waves are responsible for the significant loss of ultra-relativistic electrons, the relativistic electron population is almost unaffected. In this study, we provide a theoretical explanation for this discrepancy between previous theoretical studies and recent observations. We demonstrate that EMIC waves mainly contribute to the loss of ultra-relativistic electrons. This study significantly improves the current understanding of the electron dynamics in the Earth’s radiation belt and also can help us understand the radiation environments of the exoplanets and outer planets.
Inner magnetosphere coupling
(2017)
The dynamics of the inner magnetosphere is strongly governed by the interactions between different plasma populations that are coupled through large-scale electric and magnetic fields, currents, and wave-particle interactions. Inner magnetospheric plasma undergoes self-consistent interactions with global electric and magnetic fields. Waves excited in the inner magnetosphere from unstable particle distributions can provide energy exchange between different particle populations in the inner magnetosphere and affect the ring current and radiation belt dynamics. The ionosphere serves as an energy sink and feeds the magnetosphere back through the cold plasma outflow. The precipitating inner magnetospheric particles influence the ionosphere and upper atmospheric chemistry and affect climate. Satellite measurements and theoretical studies have advanced our understanding of the dynamics of various plasma populations in the inner magnetosphere. However, our knowledge of the coupling processes among the plasmasphere, ring current, radiation belts, global magnetic and electric fields, and plasma waves generated within these systems is still incomplete. This special issue incorporates extended papers presented at the Inner Magnetosphere Coupling III conference held 23–27 March 2015 in Los Angeles, California, USA, and includes modeling and observational contributions addressing interactions within different plasma populations in the inner magnetosphere (plasmasphere, ring current, and radiation belts), coupling between fields and plasma populations, as well as effects of the inner magnetosphere on the ionosphere and atmosphere.
We present the PINE (Plasma density in the Inner magnetosphere Neural network‐based Empirical) model ‐ a new empirical model for reconstructing the global dynamics of the cold plasma density distribution based only on solar wind data and geomagnetic indices. Utilizing the density database obtained using the NURD (Neural‐network‐based Upper hybrid Resonance Determination) algorithm for the period of 1 October 2012 to 1 July 2016, in conjunction with solar wind data and geomagnetic indices, we develop a neural network model that is capable of globally reconstructing the dynamics of the cold plasma density distribution for 2≤L≤6 and all local times. We validate and test the model by measuring its performance on independent data sets withheld from the training set and by comparing the model‐predicted global evolution with global images of He+ distribution in the Earth's plasmasphere from the IMAGE Extreme UltraViolet (EUV) instrument. We identify the parameters that best quantify the plasmasphere dynamics by training and comparing multiple neural networks with different combinations of input parameters (geomagnetic indices, solar wind data, and different durations of their time history). The optimal model is based on the 96 h time history of Kp, AE, SYM‐H, and F10.7 indices. The model successfully reproduces erosion of the plasmasphere on the nightside and plume formation and evolution. We demonstrate results of both local and global plasma density reconstruction. This study illustrates how global dynamics can be reconstructed from local in situ observations by using machine learning techniques.
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).
We present the dependence of the magnetosonic wave amplitudes both outside and inside the plasmapause on the solar wind and AE index using Van Allen Probe-A spacecraft during the time period of 1 October 2012 to 31 December 2015, based on a correlation and regression analysis. Solar wind parameters considered are the southward interplanetary magnetic field (IMF B-S), solar wind number density (N-SW), and bulk speed (V-SW). We find that the wave amplitudes outside (inside) the plasmapause are well correlated with the preceding AE, IMF B-S, and N-SW with time delays, each corresponding to 2-3 h (3-4 h), 4-5 h (3-4 h), and 2-3 h (8-9 h), while the correlation with V-SW is ambiguous both inside and outside the plasmapause. As measured by the correlation coefficient, the IMF B-S is the most influential solar wind parameter that affects the dayside wave amplitudes both outside and inside the plasmapause, while N-SW contributes to enhancing the duskside waves outside the plasmapause. The AE effect on wave amplitudes is comparable to that of IMF B-S. More interestingly, regression with time histories of the solar wind parameters and the AE index preceding the wave measurements outside the plasmapause shows significant dependence on the IMF B-S, N-SW, and AE: the region of peak coefficients is changed with time delay for IMF B-S and AE, while isolated peaks around duskside remain gradually decrease with time for N-SW. In addition, the regression with magnetosonic waves inside the plasmapause shows high coefficients around prenoon sector with preceding IMF B-S and V-SW.
Electromagnetic ion cyclotron (EMIC) waves play an important role in the dynamics of ultrarelativistic electron population in the radiation belts. However, as EMIC waves are very sporadic, developing a parameterization of such wave properties is a challenging task. Currently, there are no dynamic, activity-dependent models of EMIC waves that can be used in the long-term (several months) simulations, which makes the quantitative modeling of the radiation belt dynamics incomplete. In this study, we investigate Kp, Dst, and AE indices, solar wind speed, and dynamic pressure as possible parameters of EMIC wave presence. The EMIC waves are included in the long-term simulations (1year, including different geomagnetic activity) performed with the Versatile Electron Radiation Belt code, and we compare results of the simulation with the Van Allen Probes observations. The comparison shows that modeling with EMIC waves, parameterized by solar wind dynamic pressure, provides a better agreement with the observations among considered parameterizations. The simulation with EMIC waves improves the dynamics of ultrarelativistic fluxes and reproduces the formation of the local minimum in the phase space density profiles.
Up until recently, signatures of the ultrarelativistic electron loss driven by electromagnetic ion cyclotron (EMIC) waves in the Earth's outer radiation belt have been limited to direct or indirect measurements of electron precipitation or the narrowing of normalized pitch angle distributions in the heart of the belt. In this study, we demonstrate additional observational evidence of ultrarelativistic electron loss that can be driven by resonant interaction with EMIC waves. We analyzed the profiles derived from Van Allen Probe particle data as a function of time and three adiabatic invariants between 9 October and 29 November 2012. New local minimums in the profiles are accompanied by the narrowing of normalized pitch angle distributions and ground‐based detection of EMIC waves. Such a correlation may be indicative of ultrarelativistic electron precipitation into the Earth's atmosphere caused by resonance with EMIC waves.
Scientific Objectives of Electron Losses and Fields INvestigation Onboard Lomonosov Satellite
(2017)
The objective of the Electron Losses and Fields INvestigation on board the Lomonosov satellite ( ELFIN-L) project is to determine the energy spectrum of precipitating energetic electrons and ions and, together with other polar-orbiting and equatorial missions, to better understand the mechanisms responsible for scattering these particles into the atmosphere. This mission will provide detailed measurements of the radiation environment at low altitudes. The 400-500 km sun-synchronous orbit of Lomonosov is ideal for observing electrons and ions precipitating into the atmosphere. This mission provides a unique opportunity to test the instruments. Similar suite of instruments will be flown in the future NSF-and NASA-supported spinning CubeSat ELFIN satellites which will augment current measurements by providing detailed information on pitch-angle distributions of precipitating and trapped particles.
Significant progress has been made in recent years in understanding acceleration mechanisms in the Earth's radiation belts. In particular, a number of studies demonstrated the importance of the local acceleration by analyzing the radial profiles of phase space density (PSD) and observing building up peaks in PSD. In this study, we focus on understanding of the local loss using very similar tools. The profiles of PSD for various values of the first adiabatic invariants during the previously studied 17 January 2013 storm are presented and discussed. The profiles of PSD show clear deepening minimums consistent with the scattering by electromagnetic ion cyclotron waves. Long-term evolution shows that local minimums in PSD can persist for relatively long times. During considered interval of time the deepening minimums were observed around L* = 4 during 17 January 2013 storm and around L* = 3.5 during 1 March 2013 storm. This study shows a new method that can help identify the location, magnitude, and time of the local loss and will help quantify local loss in the future. This study also provides additional clear and definitive evidence that local loss plays a major role for the dynamics of the multi-MeV electrons.
X-ray reflectivity measurements of femtosecond laser-induced transient gratings (TG) are applied to demonstrate the spatiotemporal coherent control of thermally induced surface deformations on ultrafast time scales. Using grazing incidence x-ray diffraction we unambiguously measure the amplitude of transient surface deformations with sub-angstrom resolution. Understanding the dynamics of femtosecond TG excitations in terms of superposition of acoustic and thermal gratings makes it possible to develop new ways of coherent control in x-ray diffraction experiments. Being the dominant source of TG signal, the long-living thermal grating with spatial period. can be canceled by a second, time-delayed TG excitation shifted by Lambda/2. The ultimate speed limits of such an ultrafast x-ray shutter are inferred from the detailed analysis of thermal and acoustic dynamics in TG experiments.
We present time-resolved x-ray reflectivity measurements on laser excited coherent and incoherent surface deformations of thin metallic films. Based on a kinematical diffraction model, we derive the surface amplitude from the diffracted x-ray intensity and resolve transient surface excursions with sub-angstrom spatial precision and 70 ps temporal resolution. The analysis allows for decomposition of the surface amplitude into multiple coherent acoustic modes and a substantial contribution from incoherent phonons which constitute the sample heating. Published by AIP Publishing.
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.
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 study gadolinium thin films as a model system for ferromagnets with negative thermal expansion. Ultrashort laser pulses heat up the electronic subsystem and we follow the transient strain via ultrafast x-ray diffraction. In terms of a simple Grueneisen approach, the strain is decomposed into two contributions proportional to the thermal energy of spin and phonon subsystems. Our analysis reveals that upon femtosecond laser excitation, phonons and spins can be driven out of thermal equilibrium for several nanoseconds.
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.