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If not oriented perfectly isotropically, the strong dipole moment of polar organic semiconductor materials such as tris-(8-hydroxyquinolate)aluminum (Alq3) will lead to the buildup of a giant surface potential (GSP) and thus to a macroscopic dielectric polarization of the organic film. Despite this having been a known fact for years, the implications of such high potentials within an organic layer stack have only been studied recently. In this work, the influence of the GSP on hole injection into organic layers is investigated. Therefore, we apply a concept called dipolar doping to devices consisting of the prototypical organic materials N,N′-Di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine (NPB) as nonpolar host and Alq3 as dipolar dopant with different mixing ratios to tune the GSP. The mixtures are investigated in single-layer monopolar devices as well as bilayer metal/insulator/semiconductor structures. Characterization is done electrically using current-voltage (I-V) characteristics, impedance spectroscopy, and charge extraction by linearly increasing voltage and time of flight, as well as with ultraviolet photoelectron spectroscopy. We find a maximum in device performance for moderate to low doping concentrations of the polar species in the host. The observed behavior can be described on the basis of the Schottky effect for image-force barrier lowering, if the changes in the interface dipole, the carrier mobility, and the GSP induced by dipolar doping are taken into account.
We have investigated the structural dynamics in photoexcited 1,2-diiodotetrafluoroethane molecules (C2F4I2) in the gas phase experimentally using ultrafast electron diffraction and theoretically using FOMO-CASCI excited-state dynamics simulations. The molecules are excited by an ultraviolet femtosecond laser pulse to a state characterized by a transition from the iodine 5p perpendicular to orbital to a mixed 5p parallel to sigma hole and CF2 center dot antibonding orbital, which results in the cleavage of one of the carbon-iodine bonds. We have observed, with sub-Angstrom resolution, the motion of the nuclear wave packet of the dissociating iodine atom followed by coherent vibrations in the electronic ground state of the C2F4I radical. The radical reaches a stable classical (nonbridged) structure in less than 200 fs.
In this paper we investigate the magneto-optical (MO) and magnetic properties of bismuth iron garnet Bi3Fe5O12 thin films over a wide range of photon energies (1.6-3.5 eV) and temperatures (5-740 K). Depending on the photon energy range, the Faraday rotation (Theta(F)) and ellipticity (epsilon(F)) vary nonmonotonously with temperature. This behavior cannot be explained by a magnetization variation that can only decrease with increasing temperature. Theta(F) and epsilon(F) spectra have therefore been analyzed using a model based on two optical transitions of a diamagnetic nature, representing the tetrahedral and octahedral iron sites. Thus, the contribution of each magnetic sublattice has been extracted from the global macroscopic MO response and investigated as a function of temperature. The magnetic properties of octahedral and tetrahedral sublattices depend differently on temperature, suggesting a different anisotropy due to oxygen coordination. We have demonstrated that this relatively simple macroscopic measurement with a subsequent analysis can grant access to the information on the properties at a microscopic level. These results can advance the fundamental understanding of MO properties in multisublattice magnetic materials.
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.
Dielectric materials for electro-active (electret) and/or electro-passive (insulation) applications
(2019)
Dielectric materials for electret applications usually have to contain a quasi-permanent space charge or dipole polarization that is stable over large temperature ranges and time periods. For electrical-insulation applications, on the other hand, a quasi-permanent space charge or dipole polarization is usually considered detrimental. In recent years, however, with the advent of high-voltage direct-current (HVDC) transmission and high-voltage capacitors for energy storage, new possibilities are being explored in the area of high-voltage dielectrics. Stable charge trapping (as e.g. found in nano-dielectrics) or large dipole polarizations (as e.g. found in relaxor ferroelectrics and high-permittivity dielectrics) are no longer considered to be necessarily detrimental in electrical-insulation materials. On the other hand, recent developments in electro-electrets (dielectric elastomers), i.e. very soft dielectrics with large actuation strains and high breakdown fields, and in ferroelectrets, i.e. polymers with electrically charged cavities, have resulted in new electret materials that may also be useful for HVDC insulation systems. Furthermore, 2-dimensional (nano-particles on surfaces or interfaces) and 3-dimensional (nano-particles in the bulk) nano-dielectrics have been found to provide very good charge-trapping properties that may not only be used for more stable electrets and ferroelectrets, but also for better HVDC electrical-insulation materials with the possibility to optimize charge-transport and field-gradient behavior. In view of these and other recent developments, a first attempt will be made to review a small selection of electro-active (i.e. electret) and electro-passive (i.e. insulation) dielectrics in direct comparison. Such a comparative approach may lead to synergies in materials concepts and research methods that will benefit both areas. Furthermore, electrets may be very useful for sensing and monitoring applications in electrical-insulation systems, while high-voltage technology is essential for more efficient charging and poling of electret materials.
In the present study, the charge distribution and the charge transport across the thickness of 2- and 3-dimensional polymer nanodielectrics was investigated. Chemically surface-treated polypropylene (PP) films and low-density polyethylene nanocomposite films with 3 wt % of magnesium oxide (LDPE/MgO) served as examples of 2-D and 3-D nanodielectrics, respectively. Surface charges were deposited onto the non-metallized surfaces of the one-side metallized polymer films and found to broaden and to thus enter the bulk of the films upon thermal stimulation at suitable elevated temperatures. The resulting space-charge profiles in the thickness direction were probed by means of Piezoelectrically-generated Pressure Steps (PPSs). It was observed that the chemical surface treatment of PP which led to the formation of nano-structures or the use of bulk nanoparticles from LDPE/MgO nanocomposites enhance charge trapping on or in the respective polymer films and also reduce charge transport inside the respective samples.
Germanium oxide is a prototype network-forming oxide with pressure-induced structural changes similar to those found in crystals and amorphous silicate oxides at high pressure. Studying density and coordination changes in amorphous GeO2 allows for insight into structural changes in silicate oxides at very high pressure, with implications for the properties of planetary magmas. Here, we report the density of germanium oxide glass up to 133 GPa using the x-ray absorption technique, with very good agreement with previous experimental data at pressure below 40 GPa and recent calculation up to 140 GPa. Our data highlight four distinct compressibility domains, corresponding to changes of the local structure of GeO2. Above 80 GPa, our density data show a compressibility and bulk modulus similar to the counterpart crystal phase, and we propose that a compact distorted sixfold coordination, similar to the structural motif of the pyritelike crystalline GeO2 polymorph, is likely to be stable in that pressure range. Our density data point to a smooth continuous evolution of the average coordination for pressure above 20 GPa with persistent sixfold coordination, without sharp density or density slope discontinuities. These observations are in very good agreement with theoretical calculations and spectroscopic measurements, and our results indicate that glasses and melts may behave similarly to their high-pressure solid counterparts with comparable densities, compressibility, and possibly average coordination.
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.
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.
Charge-density rearrangements after metal-to-ligand charge-transfer excitation in an iron photosensitizer are investigated by R. M Jay, A. Fohlisch et al. in their Communication (DOI: 10.1002/anie.201904761). By using time-resolved X-ray absorption spectroscopy, surprising covalency-effects are revealed that inhibit charge-separation at the intra-molecular level. Furthermore, the underlying mechanism is proposed to be generally in effect for all commonly used photosensitizers in light-harvesting applications, which challenges the common perception of electronic charge-transfer.