2013, Bommer, Stefan, Jachalski, Sebastian, Peschka, Dirk, Seemann, Ralf, Wagner, Barbara

The morphological paths towards equilibrium droplets during the late stages of the dewetting process of a liquid film from a liquid substrate is investigated experimentally and theoretically. As liquids, short chained polystyrene (PS) and polymethyl-methacrylate (PMMA) are used, which can be considered as Newontian liquids well above their glass transition temperatures. Careful imaging of the PS/air interface of the droplets during equilibration by in situ scanning force microscopy and the PS/PMMA interface after removal of the PS droplets reveal a surprisingly deep penetration of the PS droplets into the PMMA layer. Droplets of sufficiently small volumes develop the typical lens shape and were used to extract the ratio of the PS/air and PS/PMMA surface tensions and the contact angles by comparison to theoretical exact equilibrium solutions of the liquid/liquid system. Using these results in our dynamical thin-film model we find that before the droplets reach their equilibrium they undergo several intermediate stages each with a well-defined signature in shape. Moreover, the intermediate droplet shapes are independent of the details of the initial configuration, while the time scale they are reached depend strongly on the droplet volume. This is shown by the numerical solutions of the thin-film model and demonstrated by quantitative comparison to experimental results

2016, Meca, Esteban, Münch, Andreas, Wagner, Barbara

In this study we revisit experiments by Sethuraman et al. [J. Power Sources, 195, 5062 (2010)] on the stress evolution during the lithiation/delithiation cycle of a thin film of amorphous silicon. Based on recent work that show a two-phase process of lithiation of amorphous silicon, we formulate a phase-field model coupled to elasticity in the framework of Larché-Cahn. Using an adaptive nonlinear multigrid algorithm for the finite-volume discretization of this model, our two-dimensional numerical simulations show the formation of a sharp phase boundary between the lithiated and the amorphous silicon that continues to move as a front through the thin layer. We show that our model captures the nonmonotone stress loading curve and rate dependence, as observed in experiments and connects characteristic features of the curve with the stucture formation within the layer. We take advantage of the thin film geometry and study the corresponding one-dimensional model to establish the dependence on the material parameters and obtain a comprehensive picture of the behaviour of the system.

2016, Meca, Esteban, Münch, Andreas, Wagner, Barbara

In this study we present a phase-field model that describes the process of intercalation of Li ions into a layer of an amorphous solid such as a-Si. The governing equations couple a viscous Cahn-Hilliard-Reaction model with elasticity in the framework of the Cahn-Larché system. We discuss the parameter settings and flux conditions at the free boundary that lead to the formation of phase boundaries having a sharp gradient in ion concentration between the initial state of the solid layer and the intercalated region. We carry out a matched asymptotic analysis to derive the corresponding sharp-interface model that also takes into account the dynamics of triple points where the sharp interface in the bulk of the layer intersects the free boundary. We numerically compare the interface motion predicted by the sharp-interface model with the long-time dynamics of the phase-field model.

2010, Kitavtsev, Georgy, Recke, Lutz, Wagner, Barbara

The goal of this study is the reduction of the lubrication equation, modelling thin film dynamics, onto an approximate invariant manifold. The reduction is derived for the physical situation of the late phase evolution of a dewetting thin liquid film, where arrays of droplets connected by an ultrathin film of thickness eps undergo a slow-time coarsening dynamics. With this situation in mind, we construct an asymptotic approximation of the corresponding invariant manifold, that is parametrized by a family of droplet pressures and positions, in the limit when $epsto 0$. The approach is inspired by the paper by Mielke and Zelik [Mem. Amer. Math. Soc., Vol. 198, 2009], where the center manifold reduction was carried out for a class of semilinear systems. In this study this approach is considered for quasilinear degenerate parabolic PDE's such as lubrication equations. While it has previously been shown by Glasner and Witelski [Phys. Rev. E, Vol. 67, 2003], that the system of ODEs governing the coarsening dynamics, can be obtained via formal asymptotic methods, the center manifold reduction approach presented here, pursues the rigorous justification of this asymptotic limit.

2019, Münch, Andreas, Wagner, Barbara

In this study we consider the self-consistent field theory for a dry, in- compressible polymer brush, densely grafted on a substrate, describing the average segment density of a polymer in terms of an effective chemical potential for the interaction between the segments of the polymer chain. We present a systematic singular perturbation analysis of the self-consistent field theory in the strong-stretching limit, when the length scale of the ratio of the radius of gyration of the polymer chain to the extension of the brush from the substrate vanishes. Our analysis yields, for the first time, an approximation for the average segment density that is correct to leading order in the outer scaling and resolves the boundary layer singularity at the end of the polymer brush in the strong-stretching limit. We also show that in this limit our analytical results agree increasingly well with our numerical solutions to the full model equations comprising the self-consistent field theory.

2019, Münch, Andreas, Wagner, Barbara

The most successful mean-field model to describe the collective behaviour of the large class of macromolecular polymers is the self-consistent field theory (SCFT). Still, even for the simple system of a grafted dry polymer brush, the mean-field equations have to be solved numerically. As one of very few alternatives that offer some analytical tractability the strong-stretching theory (SST) has led to explicit expressions for the effective chemical potential and consequently the free energy to promote an understanding of the underlying physics. Yet, a direct derivation of these analytical results from the SCFT model is still outstanding. In this study we present a systematic asymptotic theory based on matched asymtptotic expansions to obtain the effective chemical potential from the SCFT model for a dry polymer brush for large but finite stretching.

2017, Bergmann, Sibylle, Barragan-Yani, Daniel A., Flegel, Elke, Albe, Karsten, Wagner, Barbara

We present an atomistically informed parametrization of a phase-field model for describing the anisotropic mobility of liquid-solid interfaces in silicon. The model is derived from a consistent set of atomistic data and thus allows to directly link molecular dynamics and phase field simulations. Expressions for the free energy density, the interfacial energy and the temperature and orientation dependent interface mobility are systematically fitted to data from molecular dynamics simulations based on the Stillinger-Weber interatomic potential. The temperature-dependent interface velocity follows a Vogel-Fulcher type behavior and allows to properly account for the dynamics in the undercooled melt.

2013, Bäumchen, Oliver, Marquant, Ludovic, Blossey, Ralf, Münch, Andreas, Wagner, Barbara, Jacobs, Karin

A dewetting viscous film develops a characteristic fluid rim at its receding edge due to mass conservation. In the course of the dewetting process the rim becomes unstable via an instability of Rayleigh-Plateau type. An important difference exists between this classic instability of a liquid column and the rim instability in the thin film as the growth of the rim is continuously fueled by the receding film. We explain how the development and macroscopic morphology of the rim instability are controlled by the slip of the film on the substrate. A single thin-film model captures quantitatively the characteristics of the evolution of the rim observed in our experiments.

2010, Kitavtsev, Georgy, Recke, Lutz, Wagner, Barbara

In this paper the linear stability properties of the steady states of a no-slip lubrication equation are studied. The steady states are configurations of droplets and arise during the late-phase dewetting process under the influence of both destabilizing van der Waals and stabilizing Born intermolecular forces, which in turn give rise to the minimum thickness eps of the remaining film connecting the droplets. The goal of this paper is to give an asymptotic description of the eigenvalues and eigenfunctions of the problem, linearized about the one-droplet solutions, as epsto 0. For this purpose, corresponding asymptotic eigenvalue problems with piecewise constant coefficients are constructed, such that their eigenvalue asymptotics can be determined analytically. A comparison with numerically computed eigenvalues and eigenfunctions shows good agreement with the asymptotic results and the existence of a spectrum gap to a single exponentially small eigenvalue for sufficiently small eps.

2007, Afanasiev, Konstantin, Münch, Andreas, Wagner, Barbara

In this paper the drag-out problem for shear-thinning liquids at variable inclination angle is considered. For this free boundary problem dimension-reduced lubrication equations are derived for the most commonly used viscosity models, namely, the power-law, Ellis and Carreau model. For the resulting lubrication models a system of ordinary differential equation governing the steady state solutions is obtained. Phase plane analysis is used to characterize the type of possible steady state solutions and their dependence on the rheological parameters.