Refine
Has Fulltext
- no (117)
Year of publication
- 2021 (117) (remove)
Document Type
- Article (117) (remove)
Language
- English (117) (remove)
Is part of the Bibliography
- yes (117)
Keywords
- diffusion (6)
- MHD (5)
- anomalous diffusion (4)
- intergalactic medium (4)
- methods: numerical (4)
- cosmic rays (3)
- organic solar cells (3)
- quasars: absorption lines (3)
- stars: massive (3)
- stars: variables: general (3)
Institute
- Institut für Physik und Astronomie (117) (remove)
State-of-the-art organic solar cells exhibit power conversion efficiencies of 18% and above. These devices benefit from the suppression of free charge recombination with regard to the Langevin limit of charge encounter in a homogeneous medium. It is recognized that the main cause of suppressed free charge recombination is the reformation and resplitting of charge-transfer (CT) states at the interface between donor and acceptor domains. Here, we use kinetic Monte Carlo simulations to understand the interplay between free charge motion and recombination in an energetically disordered phase-separated donor-acceptor blend. We identify conditions for encounter-dominated and resplitting-dominated recombination. In the former regime, recombination is proportional to mobility for all parameters tested and only slightly reduced with respect to the Langevin limit. In contrast, mobility is not the decisive parameter that determines the nongeminate recombination coefficient, k(2), in the latter case, where k2 is a sole function of the morphology, CT and charge-separated (CS) energetics, and CT-state decay properties. Our simulations also show that free charge encounter in the phase-separated disordered blend is determined by the average mobility of all carriers, while CT reformation and resplitting involves mostly states near the transport energy. Therefore, charge encounter is more affected by increased disorder than the resplitting of the CT state. As a consequence, for a given mobility, larger energetic disorder, in combination with a higher hopping rate, is preferred. These findings have implications for the understanding of suppressed recombination in solar cells with nonfullerene acceptors, which are known to exhibit lower energetic disorder than that of fullerenes.
In contrast to the common conception that the interfacial energy-level alignment is affixed once the interface is formed, we demonstrate that heterojunctions between organic semiconductors and metal-halide perovskites exhibit huge energy-level realignment during photoexcitation. Importantly, the photoinduced level shifts occur in the organic component, including the first molecular layer in direct contact with the perovskite. This is caused by charge-carrier accumulation within the organic semiconductor under illumination and the weak electronic coupling between the junction components.
We investigate the transition from incoherence to global collective motion in a three-dimensional swarming model of agents with helical trajectories, subject to noise and global coupling. Without noise this model was recently proposed as a generalization of the Kuramoto model and it was found that alignment of the velocities occurs discontinuously for arbitrarily small attractive coupling. Adding noise to the system resolves this singular limit and leads to a continuous transition, either to a directed collective motion or to center-of-mass rotations.
Reciprocal space slicing
(2021)
An experimental technique that allows faster assessment of out-of-plane strain dynamics of thin film heterostructures via x-ray diffraction is presented. In contrast to conventional high-speed reciprocal space-mapping setups, our approach reduces the measurement time drastically due to a fixed measurement geometry with a position-sensitive detector. This means that neither the incident (ω) nor the exit (2θ) diffraction angle is scanned during the strain assessment via x-ray diffraction. Shifts of diffraction peaks on the fixed x-ray area detector originate from an out-of-plane strain within the sample. Quantitative strain assessment requires the determination of a factor relating the observed shift to the change in the reciprocal lattice vector. The factor depends only on the widths of the peak along certain directions in reciprocal space, the diffraction angle of the studied reflection, and the resolution of the instrumental setup. We provide a full theoretical explanation and exemplify the concept with picosecond strain dynamics of a thin layer of NbO2.
Surface melting of the Greenland Ice Sheet contributes a large amount to current and future sea level rise. Increased surface melt may lower the reflectivity of the ice sheet surface and thereby increase melt rates: the so-called melt-albedo feedback describes this self-sustaining increase in surface melting. In order to test the effect of the melt-albedo feedback in a prognostic ice sheet model, we implement dEBM-simple, a simplified version of the diurnal Energy Balance Model dEBM, in the Parallel Ice Sheet Model (PISM). The implementation includes a simple representation of the melt-albedo feedback and can thereby replace the positive-degree-day melt scheme. Using PISM-dEBM-simple, we find that this feedback increases ice loss through surface warming by 60 % until 2300 for the high-emission scenario RCP8.5 when compared to a scenario in which the albedo remains constant at its present-day values. With an increase of 90 % compared to a fixed-albedo scenario, the effect is more pronounced for lower surface warming under RCP2.6. Furthermore, assuming an immediate darkening of the ice surface over all summer months, we estimate an upper bound for this effect to be 70 % in the RCP8.5 scenario and a more than 4-fold increase under RCP2.6. With dEBM-simple implemented in PISM, we find that the melt-albedo feedback is an essential contributor to mass loss in dynamic simulations of the Greenland Ice Sheet under future warming.
Constraints on the time-scales of quasar activity are key to understanding the formation and growth of supermassive black holes (SMBHs), quasar triggering mechanisms, and possible feedback effects on their host galaxies. However, observational estimates of this so-called quasar lifetime are highly uncertain (t(Q) similar to 10(4)-10(9) yr), because most methods are indirect and involve many model-dependent assumptions. Direct evidence of earlier activity is gained from the higher ionization state of the intergalactic medium (IGM) in the quasar environs, observable as enhanced Ly alpha transmission in the so-called proximity zone. Due to the similar to 30 Myr equilibration time-scale of He II in the z similar to 3 IGM, the size of the He II proximity zone depends on the time the quasar had been active before our observation t(on) <= t(Q), enabling up to +/- 0.2 dex precise measurements of individual quasar on-times that are comparable to the e-folding time-scale t(S) <= 44 Myr of SMBH growth. Here we present the first statistical sample of 13 quasars whose accurate and precise systemic redshifts allow for measurements of sufficiently precise He II quasar proximity zone sizes between similar or equal to 2 and similar or equal to 15 proper Mpc from science-grade Hubble Space Telescope (HST) spectra. Comparing these sizes to predictions from cosmological hydrodynamical simulations post-processed with 1D radiative transfer, we infer a broad range of quasar on-times from t(on) less than or similar to 1Myr to t(on) > 30 Myr that does not depend on quasar luminosity, black hole mass, or Eddington ratio. These results point to episodic quasar activity over a long duty cycle, but do not rule out substantial SMBH growth during phases of radiative inefficiency or obscuration.
Phase equilibria that are relevant for the growth of Bi2MO4 have been studied experimentally, and the ternary phase diagrams of Bi2O3-PdO2-Pd and Bi2O3-Cu2O-CuO and its isopleth section Bi2O3-CuO were redetermined. It is shown that every melting and crystallization process is always accompanied by a redox process at the phase boundary and that for both title compounds, the valence of the transition metal is lowered during melting. Vice versa, during crystal growth, O-2 must be transported through the melt to the phase boundary. Based on these new insights provided by our thermodynamic studies, Bi2CuO4 single crystals with a length of up to 7 cm and a diameter of 6 mm were grown by the OFZ technique to be used for investigations of magnetic, electronic and thermal transport properties. The grown crystals were characterized by powder X-ray diffraction, Laue, magnetization and specific heat measurements.
Increasing greenhouse gas emissions are likely to impact not only natural systems but economies worldwide. If these impacts alter future economic development, the financial losses will be significantly higher than the mere direct damages. So far, potentially aggravating investment responses were considered negligible. Here we consistently incorporate an empirically derived temperature-growth relation into the simple integrated assessment model DICE. In this framework we show that, if in the next eight decades varying temperatures impact economic growth as has been observed in the past three decades, income is reduced by similar to 20% compared to an economy unaffected by climate change. Hereof similar to 40% are losses due to growth effects of which similar to 50% result from reduced incentive to invest. This additional income loss arises from a reduced incentive for future investment in anticipation of a reduced return and not from an explicit climate protection policy. Under economically optimal climate-change mitigation, however, optimal investment would only be reduced marginally as mitigation efforts keep returns high.
'Complex systems are information processors' is a statement that is frequently made. Here we argue for the distinction between information processing-in the sense of encoding and transmitting a symbolic representation-and the formation of correlations (pattern formation/self-organisation). The study of both uses tools from information theory, but the purpose is very different in each case: explaining the mechanisms and understanding the purpose or function in the first case, versus data analysis and correlation extraction in the latter. We give examples of both and discuss some open questions. The distinction helps focus research efforts on the relevant questions in each case.
A detailed investigation of the energy levels of perylene-3,4,9,10-tetracarboxylic tetraethylester as a representative compound for the whole family of perylene esters was performed. It was revealed via electrochemical measurements that one oxidation and two reductions take place. The bandgaps determined via the electrochemical approach are in good agreement with the optical bandgap obtained from the absorption spectra via a Tauc plot. In addition, absorption spectra in dependence of the electrochemical potential were the basis for extensive quantum-chemical calculations of the neutral, monoanionic, and dianionic molecules. For this purpose, calculations based on density functional theory were compared with post-Hartree-Fock methods and the CAM-B3LYP functional proved to be the most reliable choice for the calculation of absorption spectra. Furthermore, spectral features found experimentally could be reproduced with vibronic calculations and allowed to understand their origins. In particular, the two lowest energy absorption bands of the anion are not caused by absorption of two distinct electronic states, which might have been expected from vertical excitation calculations, but both states exhibit a strong vibronic progression resulting in contributions to both bands.