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- ItemShort-Range Cooperative Slow-down of Water Solvation Dynamics Around SO42--Mg2+ Ion Pairs(Washington, DC : American Chemical Society, 2022) Kundu, Achintya; Mamatkulov, Shavkat I.; Brünig, Florian N.; Bonthuis, Douwe Jan; Netz, Roland R.; Elsaesser, Thomas; Fingerhut, Benjamin P.The presence of ions affects the structure and dynamics of water on a multitude of length and time scales. In this context, pairs of Mg2+ and SO42- ions in water constitute a prototypical system for which conflicting pictures of hydration geometries and dynamics have been reported. Key issues are the molecular pair and solvation shell geometries, the spatial range of electric interactions, and their impact on solvation dynamics. Here, we introduce asymmetric SO42- stretching vibrations as new and most specific local probes of solvation dynamics that allow to access ion hydration dynamics at the dilute concentration (0.2 M) of a native electrolyte environment. Highly sensitive heterodyne 2D-IR spectroscopy in the fingerprint region of the SO42- ions around 1100 cm-1 reveals a specific slow-down of solvation dynamics for hydrated MgSO4 and for Na2SO4 in the presence of Mg2+ ions, which manifests as a retardation of spectral diffusion compared to aqueous Na2SO4 solutions in the absence of Mg2+ ions. Extensive molecular dynamics and density functional theory QM/MM simulations provide a microscopic view of the observed ultrafast dephasing and hydration dynamics. They suggest a molecular picture where the slow-down of hydration dynamics arises from the structural peculiarities of solvent-shared SO42--Mg2+ ion pairs.
- 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
- ItemEngineering Micropatterned Dry Adhesives: From Contact Theory to Handling Applications(Weinheim : Wiley-VCH, 2018) Hensel, René; Moh, Karsten; Arzt, EduardReversible adhesion is the key functionality to grip, place, and release objects nondestructively. Inspired by nature, micropatterned dry adhesives are promising candidates for this purpose and have attracted the attention of research groups worldwide. Their enhanced adhesion compared to nonpatterned surfaces is frequently demonstrated. An important conclusion is that the contact mechanics involved is at least as important as the surface energy and chemistry. In this paper, the roles of the contact geometry and mechanical properties are reviewed. With a focus on applications, the effects of substrate roughness and of temperature variations, and the long-term performance of micropatterned adhesives are discussed. The paper provides a link between the current, detailed understanding of micropatterned adhesives and emerging applications.
- ItemSemitransparent Perovskite Solar Cells with an Evaporated Ultra-Thin Perovskite Absorber(Weinheim : Wiley-VCH, 2023) Zhang, Zongbao; Ji, Ran; Jia, Xiangkun; Wang, Shu‐Jen; Deconinck, Marielle; Siliavka, Elena; Vaynzof, YanaMetal halide perovskites are of great interest for application in semitransparent solar cells due to their tunable bandgap and high performance. However, fabricating high-efficiency perovskite semitransparent devices with high average visible transmittance (AVT) is challenging because of their high absorption coefficient. Here, a co-evaporation process is adopted to fabricate ultra-thin CsPbI3 perovskite films. The smooth surface and orientated crystal growth of the evaporated perovskite films make it possible to achieve 10 nm thin films with compact and continuous morphology without pinholes. When integrated into a p-i-n device structure of glass/ITO/PTAA/perovskite/PCBM/BCP/Al/Ag with an optimized transparent electrode, these ultra-thin layers result in an impressive open-circuit voltage (VOC) of 1.08 V and a fill factor (FF) of 80%. Consequently, a power conversion efficiency (PCE) of 3.6% with an AVT above 50% is demonstrated, which is the first report for a perovskite device of a 10 nm active layer thickness with high VOC, FF and AVT. These findings demonstrate that deposition by thermal evaporation makes it possible to form compact ultra-thin perovskite films, which are of great interest for future smart windows, light-emitting diodes, and tandem device applications.
- ItemTransparent Power-Generating Windows Based on Solar-Thermal-Electric Conversion(Weinheim : Wiley-VCH, 2021) Zhang, Qihao; Huang, Aibin; Ai, Xin; Liao, Jincheng; Song, Qingfeng; Reith, Heiko; Cao, Xun; Fang, Yueping; Schierning, Gabi; Nielsch, Kornelius; Bai, Shengqiang; Chen, LidongIntegrating transparent solar-harvesting systems into windows can provide renewable on-site energy supply without altering building aesthetics or imposing further design constraints. Transparent photovoltaics have shown great potential, but the increased transparency comes at the expense of reduced power-conversion efficiency. Here, a new technology that overcomes this limitation by combining solar-thermal-electric conversion with a material's wavelength-selective absorption is presented. A wavelength-selective film consisting of Cs0.33WO3 and resin facilitates high visible-light transmittance (up to 88%) and outstanding ultraviolet and infrared absorbance, thereby converting absorbed light into heat without sacrificing transparency. A prototype that couples the film with thermoelectric power generation produces an extraordinary output voltage of ≈4 V within an area of 0.01 m2 exposed to sunshine. Further optimization design and experimental verification demonstrate high conversion efficiency comparable to state-of-the-art transparent photovoltaics, enriching the library of on-site energy-saving and transparent power generation.
- ItemSilane-Mediated Expansion of Domains in Si-Doped κ-Ga2O3 Epitaxy and its Impact on the In-Plane Electronic Conduction(Weinheim : Wiley-VCH, 2022) Mazzolini, Piero; Fogarassy, Zsolt; Parisini, Antonella; Mezzadri, Francesco; Diercks, David; Bosi, Matteo; Seravalli, Luca; Sacchi, Anna; Spaggiari, Giulia; Bersani, Danilo; Bierwagen, Oliver; Janzen, Benjamin Moritz; Marggraf, Marcella Naomi; Wagner, Markus R.; Cora, Ildiko; Pécz, Béla; Tahraoui, Abbes; Bosio, Alessio; Borelli, Carmine; Leone, Stefano; Fornari, RobertoUnintentionally doped (001)-oriented orthorhombic κ-Ga2O3 epitaxial films on c-plane sapphire substrates are characterized by the presence of ≈ 10 nm wide columnar rotational domains that can severely inhibit in-plane electronic conduction. Comparing the in- and out-of-plane resistance on well-defined sample geometries, it is experimentally proved that the in-plane resistivity is at least ten times higher than the out-of-plane one. The introduction of silane during metal-organic vapor phase epitaxial growth not only allows for n-type Si extrinsic doping, but also results in the increase of more than one order of magnitude in the domain size (up to ≈ 300 nm) and mobility (highest µ ≈ 10 cm2V−1s−1, with corresponding lowest ρ ≈ 0.2 Ωcm). To qualitatively compare the mean domain dimension in κ-Ga2O3 epitaxial films, non-destructive experimental procedures are provided based on X-ray diffraction and Raman spectroscopy. The results of this study pave the way to significantly improved in-plane conduction in κ-Ga2O3 and its possible breakthrough in new generation electronics. The set of cross-linked experimental techniques and corresponding interpretation here proposed can apply to a wide range of material systems that suffer/benefit from domain-related functional properties.
- ItemCurrent State-of-the-Art in the Interface/Surface Modification of Thermoelectric Materials(Weinheim : Wiley-VCH, 2021) He, Shiyang; Lehmann, Sebastian; Bahrami, Amin; Nielsch, KorneliusThermoelectric (TE) materials are prominent candidates for energy converting applications due to their excellent performance and reliability. Extensive efforts for improving their efficiency in single-/multi-phase composites comprising nano/micro-scale second phases are being made. The artificial decoration of second phases into the thermoelectric matrix in multi-phase composites, which is distinguished from the second-phase precipitation occurring during the thermally equilibrated synthesis of TE materials, can effectively enhance their performance. Theoretically, the interfacial manipulation of phase boundaries can be extended to a wide range of materials. High interface densities decrease thermal conductivity when nano/micro-scale grain boundaries are obtained and certain electronic structure modifications may increase the power factor of TE materials. Based on the distribution of second phases on the interface boundaries, the strategies can be divided into discontinuous and continuous interfacial modifications. The discontinuous interfacial modifications section in this review discusses five parts chosen according to their dispersion forms, including metals, oxides, semiconductors, carbonic compounds, and MXenes. Alternatively, gas- and solution-phase process techniques are adopted for realizing continuous surface changes, like the core–shell structure. This review offers a detailed analysis of the current state-of-the-art in the field, while identifying possibilities and obstacles for improving the performance of TE materials.
- 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.