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- ItemRevealing all states of dewetting of a thin gold layer on a silicon surface by nanosecond laser conditioning(Amsterdam : Elsevier, 2021) Ernst, Owen C.; Uebel, David; Kayser, Stefan; Lange, Felix; Teubner, Thomas; Boeck, TorstenDewetting is a ubiquitous phenomenon which can be applied to the laser synthesis of nanoparticles. A classical spinodal dewetting process takes place in four successive states, which differ from each other in their morphology. In this study all states are revealed by interaction of pulsed nanosecond UV laser light with thin gold layers with thicknesses between 1 nm and 10 nm on (100) silicon wafers. The specific morphologies of the dewetting states are discussed with particular emphasis on the state boundaries. The main parameter determining which state is formed is not the duration for which the gold remains liquid, but rather the input energy provided by the laser. This shows that each state transition has a separate measurable activation energy. The temperature during the nanosecond pulses and the duration during which the gold remains liquid was determined by simulation using the COMSOL Multiphysics® software package. Using these calculations, an accurate local temperature profile and its development over time was simulated. An analytical study of the morphologies and formed structures was performed using Minkowski measures. With aid of this tool, the laser induced structures were compared with thermally annealed samples, with perfectly ordered structures and with perfectly random structures. The results show that both, structures of the laser induced and the annealed samples, strongly resemble the perfectly ordered structures. This reveals a close relationship between these structures and suggests that the phenomenon under investigation is indeed a spinodal dewetting generated by an internal material wave function. The purposeful generation of these structures and the elucidation of the underlying mechanism of dewetting by short pulse lasers may assist the realisation of various technical elements such as nanowires in science and industry. © 2020
- ItemElectron beam induced dehydrogenation of MgH2 studied by VEELS(Cham : Springer International Publishing AG, 2016) Surrey, Alexander; Schultz, Ludwig; Rellinghaus, BerndNanosized or nanoconfined hydrides are promising materials for solid-state hydrogen storage. Most of these hydrides, however, degrade fast during the structural characterization utilizing transmission electron microscopy (TEM) upon the irradiation with the imaging electron beam due to radiolysis. We use ball-milled MgH2 as a reference material for in-situ TEM experiments under low-dose conditions to study and quantitatively understand the electron beam-induced dehydrogenation. For this, valence electron energy loss spectroscopy (VEELS) measurements are conducted in a monochromated FEI Titan3 80–300 microscope. From observing the plasmonic absorptions it is found that MgH2 successively converts into Mg upon electron irradiation. The temporal evolution of the spectra is analyzed quantitatively to determine the thickness-dependent, characteristic electron doses for electron energies of both 80 and 300 keV. The measured electron doses can be quantitatively explained by the inelastic scattering of the incident high-energy electrons by the MgH2 plasmon. The obtained insights are also relevant for the TEM characterization of other hydrides.
- ItemMultistatic Specular Meteor Radar Network in Peru: System Description and Initial Results(Malden, Mass. : American Geophysical Union, 2021) Chau, J.L.; Urco, J.M.; Vierinen, J.; Harding, B.J.; Clahsen, M.; Pfeffer, N.; Kuyeng, K.M.; Milla, M.A.; Erickson, P.J.The mesosphere and lower thermosphere (MLT) region is dominated globally by dynamics at various scales: planetary waves, tides, gravity waves, and stratified turbulence. The latter two can coexist and be significant at horizontal scales less than 500 km, scales that are difficult to measure. This study presents a recently deployed multistatic specular meteor radar system, SIMONe Peru, which can be used to observe these scales. The radars are positioned at and around the Jicamarca Radio Observatory, which is located at the magnetic equator. Besides presenting preliminary results of typically reported large-scale features, like the dominant diurnal tide at low latitudes, we show results on selected days of spatially and temporally resolved winds obtained with two methods based on: (a) estimation of mean wind and their gradients (gradient method), and (b) an inverse theory with Tikhonov regularization (regularized wind field inversion method). The gradient method allows improved MLT vertical velocities and, for the first time, low-latitude wind field parameters such as horizontal divergence and relative vorticity. The regularized wind field inversion method allows the estimation of spatial structure within the observed area and has the potential to outperform the gradient method, in particular when more detections are available or when fine adaptive tuning of the regularization factor is done. SIMONe Peru adds important information at low latitudes to currently scarce MLT continuous observing capabilities. Results contribute to studies of the MLT dynamics at different scales inherently connected to lower atmospheric forcing and E-region dynamo related ionospheric variability.
- ItemBio-inspired deposition of electrochemically exfoliated graphene layers for electrical resistance heating applications(Bristol : IOP Publishing, 2020-12-4) Utech, Toni; Pötschke, Petra; Simon, Frank; Janke, Andreas; Kettner, Hannes; Paiva, Maria; Zimmerer, CordeliaElectrochemically exfoliated graphene (eeG) layers possess a variety of potential applications, e.g. as susceptor material for contactless induction heating in dynamic electro-magnetic fields, and as flexible and transparent electrode or resistivity heating elements. Spray coating of eeG dispersions was investigated in detail as a simple and fast method to deposit both, thin conducting layers and ring structures on polycarbonate substrates. The spray coating process was examined by systematic variation of dispersion concentration and volume applied to heated substrates. Properties of the obtained layers were characterized by UV-VIS spectroscopy, SEM and Confocal Scanning Microscopy. Electrical conductivity of eeG ring structures was measured using micro-four-point measurements. Modification of eeG with poly(dopamine) and post-thermal treatment yields in the reduction of the oxidized graphene proportion, an increase in electrical conductivity, and mechanical stabilization of the deposited thin layers. The chemical composition of modified eeG layer was analyzed via x-ray photoelectron spectroscopy pointing to the reductive behavior of poly(dopamine). Application oriented experiments demonstrate the direct electric current heating (Joule-Heating) effect of spray-coated eeG layers.
- ItemDesign of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries(London [u.a.] : RSC, 2022) Arnold, Stefanie; Gentile, Antonio; Li, Yunjie; Wang, Qingsong; Marchionna, Stefano; Ruffo, Riccardo; Presser, VolkerDue to their versatile properties and excellent electrical conductivity, MXenes have become attractive materials for alkali metal-ion batteries. However, as the capacity is limited to lower values due to the intercalation mechanism, these materials can hardly keep up in the ever-fast-growing community of battery research. Antimony has a promisingly high theoretical sodiation capacity characterized by an alloying reaction. The main drawback of this type of battery material is related to the high volume changes during cycling, often leading to electrode cracking and pulverization, resulting in poor electrochemical performance. A synergistic effect of combing antimony and MXene can be expected to obtain an optimized electrochemical system to overcome capacity fading of antimony while taking advantage of MXene charge storage ability. In this work, variation of the synthesis parameters and material design strategy have been dedicated to achieving the optimized antimony/MXene hybrid electrodes for high-performance sodium-ion batteries. The optimized performance does not align with the highest amount of antimony, the smallest nanoparticles, or the largest interlayer distance of MXene but with the most homogeneous distribution of antimony and MXene while both components remain electrochemically addressable. As a result, the electrode with 40 mass% MXene, not previously expanded, etched with 5 mass% HF and 60% antimony synthesized on the surfaces of MXene emerged as the best electrode. We obtained a high reversible capacity of 450 mA h g−1 at 0.1 A g−1 with a capacity retention of around 96% after 100 cycles with this hybrid material. Besides the successful cycling stability, this material also exhibits high rate capability with a capacity of 365 mA h g−1 at 4 A g−1. In situ XRD measurements and post mortem analysis were used to investigate the reaction mechanism.
- ItemLarge-area wet-chemical deposition of nanoporous tungstic silica coatings(London [u.a.] : RSC, 2015) Nielsen, K.H.; Wondraczek, K.; Schubert, U.S.; Wondraczek, L.We report on a facile procedure for synthesis of nanoporous coatings of tungstic silica through wet-chemical deposition and post-treatment of tungsten-doped potassium silicate solutions. The process relies on an aqueous washing and ion exchange step where dispersed potassium salt deposits are removed from a 150 nm silicate gel layer. Through an adjustment of the pH value of the washing agent within the solubility regime of a tungstic salt precursor, the tungsten content of the remaining nanostructured coating can be controlled. We propose this route as a universal approach for the deposition of large-area coatings of nanoporous silica with the potential for incorporating a broad variety of other dopant species. As for the present case, we observe, on the one hand, antireflective properties which enable the reduction of reflection losses from float glass by up to 3.7 percent points. On the other hand, the incorporation of nanoscale tungstic precipitates provides a lever for tailoring the coating hydrophilicity and, eventually, also surface acidity. This may provide a future route for combining optical performance with anti-fouling functionality.
- ItemNiobium carbide nanofibers as a versatile precursor for high power supercapacitor and high energy battery electrodes(London [u.a.] : RSC, 2016) Tolosa, Aura; Krüner, Benjamin; Fleischmann, Simon; Jäckel, Nicolas; Zeiger, Marco; Aslan, Mesut; Grobelsek, Ingrid; Presser, VolkerThis study presents electrospun niobium carbide/carbon (NbC/C) hybrid nanofibers, with an average diameter of 69 ± 30 nm, as a facile precursor to derive either highly nanoporous niobium carbide-derived carbon (NbC–CDC) fibers for supercapacitor applications or niobium pentoxide/carbon (Nb2O5/C) hybrid fibers for battery-like energy storage. In all cases, the electrodes consist of binder-free and free-standing nanofiber mats that can be used without further conductive additives. Chlorine gas treatment conformally transforms NbC nanofiber mats into NbC–CDC fibers with a specific surface area of 1508 m2 g−1. These nanofibers show a maximum specific energy of 19.5 W h kg−1 at low power and 7.6 W h kg−1 at a high specific power of 30 kW kg−1 in an organic electrolyte. CO2 treatment transforms NbC into T-Nb2O5/C hybrid nanofiber mats that provide a maximum capacity of 156 mA h g−1. The presence of graphitic carbon in the hybrid nanofibers enabled high power handling, maintaining 50% of the initial energy storage capacity at a high rate of 10 A g−1 (64 C-rate). When benchmarked for an asymmetric full-cell, a maximum specific energy of 86 W h kg−1 was obtained. The high specific power for both systems, NbC–CDC and T-Nb2O5/C, resulted from the excellent charge propagation in the continuous nanofiber network and the high graphitization of the carbon structure.
- ItemEffects of PNDIT2 end groups on aggregation, thin film structure, alignment and electron transport in field-effect transistors(London [u.a.] : RSC, 2016) Matsidik, Rukiya; Luzio, Alessandro; Hameury, Sophie; Komber, Hartmut; McNeill, Christopher R.; Caironi, Mario; Sommer, MichaelTo develop greener protocols toward the sustainable production of conjugated polymers, we combine the advantages of atom-economic direct arylation polycondensation (DAP) with those of the green solvent 2-methyltetrahydrofuran (MeTHF). The n-type copolymer PNDIT2 is synthesized from unsubstituted bithiophene (T2) and 2,6-dibromonapthalene diimide (NDIBr2) under simple DAP conditions in MeTHF. Extensive optimization is required to suppress nucleophilic substitution of NDIBr end groups, which severely limits molar mass. Different carboxylic acids, bases, palladium precursors and ligands are successfully screened to enable quantitative yield and satisfyingly high molar masses up to Mn,SEC ∼ 20 kDa. In contrast to PNDIT2 made via DAP in toluene with tolyl-chain termini, nucleophilic substitution of NDIBr chain ends in MeTHF finally leads to NDI-OH termination. The influence of different chain termini on the optical, thermal, structural and electronic properties of PNDIT2 is investigated. For samples with identical molecular weight, OH-termination leads to slightly reduced aggregation in solution and bulk crystallinity, a decreased degree of alignment in directionally deposited films, and a consequently reduced, but not compromised, electron mobility with promising values still close to 0.9 cm2 V−1 s−1.
- ItemInvestigating the electrochemical stability of Li7La3Zr2O12 solid electrolytes using field stress experiments(London [u.a.] : RSC, 2021) Smetaczek, Stefan; Pycha, Eva; Ring, Joseph; Siebenhofer, Matthäus; Ganschow, Steffen; Berendts, Stefan; Nenning, Andreas; Kubicek, Markus; Rettenwander, Daniel; Limbeck, Andreas; Fleig, JürgenCubic Li7La3Zr2O12 (LLZO) garnets are among the most promising solid electrolytes for solid-state batteries with the potential to exceed conventional battery concepts in terms of energy density and safety. The electrochemical stability of LLZO is crucial for its application, however, controversial reports in the literature show that it is still an unsettled matter. Here, we investigate the electrochemical stability of LLZO single crystals by applying electric field stress via macro- and microscopic ionically blocking Au electrodes in ambient air. Induced material changes are subsequently probed using various locally resolved analysis techniques, including microelectrode electrochemical impedance spectroscopy (EIS), laser induced breakdown spectroscopy (LIBS), laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS), and microfocus X-ray diffraction (XRD). Our experiments indicate that LLZO decomposes at 4.1–4.3 V vs. Li+/Li, leading to the formation of Li-poor phases like La2Zr2O7 beneath the positively polarized electrode. The reaction is still on-going even after several days of polarization, indicating that no blocking interfacial layer is formed. The decomposition can be observed at elevated as well as room temperature and suggests that LLZO is truly not compatible with high voltage cathode materials.
- ItemTuning the magneto-optical response of TbPc2 single molecule magnets by the choice of the substrate(London [u.a.] : RSC, 2015) Robaschik, Peter; Fronk, Michael; Toader, Marius; Klyatskaya, Svetlana; Ganss, Fabian; Siles, Pablo F.; Schmidt, Oliver G.; Albrecht, Manfred; Hietschold, Michael; Ruben, Mario; Zahn, Dietrich R.T.; Salvan, GeorgetaIn this work, we investigated the magneto-optical response of thin films of TbPc2 on substrates which are relevant for (spin) organic field effect transistors (SiO2) or vertical spin valves (Co) in order to explore the possibility of implementing TbPc2 in magneto-electronic devices, the functionality of which includes optical reading. The optical and magneto-optical properties of TbPc2 thin films prepared by organic molecular beam deposition (OMBD) on silicon substrates covered with native oxide were investigated by variable angle spectroscopic ellipsometry (VASE) and magneto-optical Kerr effect (MOKE) spectroscopy at room temperature. The magneto-optical activity of the TbPc2 films can be significantly enhanced by one to two orders of magnitude upon changing the molecular orientation (from nearly standing molecules on SiO2/Si substrates to nearly lying molecules on perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) templated SiO2/Si substrates) or by using metallic ferromagnetic substrates (Co).
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