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    Revealing 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, Torsten
    Dewetting 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
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    A discussion of the cell voltage during discharge of an intercalation electrode for various C-rates based on non-equilibrium thermodynamics and numerical simulations
    (Bristol : IOP Publishing, 2020) Landstorfer, Manuel
    In this work we discuss the modeling procedure and validation of a non-porous intercalation half-cell during galvanostatic discharge. The modeling is based on continuum thermodynamics with non-equilibrium processes in the active intercalation particle, the electrolyte, and the common interface where the intercalation reaction Li+ + e- ↔ Li occurs. The model is in detail investigated and discussed in terms of scalings of the non-equilibrium parameters, i.e. the diffusion coefficients DA and DE of the active phase and the electrolyte, conductivity sA and sE of both phases, and the exchange current density e0L, with numerical solutions of the underlying PDE system. The current density i as well as all non-equilibrium parameters are scaled s with respect to the 1-C current density iC A of the intercalation electrode. We compute then numerically the cell voltage E as function of the capacity Q and the C-rate Ch. Within a hierarchy of approximations we provide computations of E(Q) for various scalings of the diffusion coefficients, the conductivities and the exchange current density. For the later we provide finally a discussion for possible concentration dependencies. © The Author(s) 2019. Published by ECS.
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    Modeling Polycrystalline Electrode-electrolyte Interfaces: The Differential Capacitance
    (Bristol : IOP Publishing, 2020) Müller, Rüdiger; Fuhrmann, Jürgen; Landstorfer, Manuel
    We present and analyze a model for polycrystalline electrode surfaces based on an improved continuum model that takes finite ion size and solvation into account. The numerical simulation of finite size facet patterns allows to study two limiting cases: While for facet size diameter dfacet →0 we get the typical capacitance of a spatially homogeneous but possible amorphous or liquid surface, in the limit 1[nm] < dfacet, an ensemble of non-interacting single crystal surfaces is approached. Already for moderate size of the facet diameters, the capacitance is remarkably well approximated by the classical approach of adding the single crystal capacities of the contributing facets weighted by their respective surface fraction. As a consequence, the potential of zero charge is not necessarily attained at a local minimum of capacitance, but might be located at a local capacitance maximum instead. Moreover, the results show that surface roughness can be accurately taken into account by multiplication of the ideally flat polycrystalline surface capacitance with a single factor. In particular, we find that the influence of the actual geometry of the facet pattern in negligible and our theory opens the way to a stochastic description of complex real polycrystal surfaces. © 2020 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited.