Modelling the evaporation of thin films of colloidal suspensions using Dynamical Density Functional Theory

Recent experiments have shown that various structures may be formed during the evaporative dewetting of thin films of colloidal suspensions. Nano-particle deposits of strongly branched `flower-like', labyrinthine and network structures are observed. They are caused by the different transport processes and the rich phase behaviour of the system. We develop a model for the system, based on a dynamical density functional theory, which reproduces these structures. The model is employed to determine the influences of the solvent evaporation and of the diffusion of the colloidal particles and of the liquid over the surface. Finally, we investigate the conditions needed for `liquid-particle' phase separation to occur and discuss its effect on the self-organised nano-structures

Depinning of three-dimensional drops from wettability defects

Substrate defects crucially influence the onset of sliding drop motion under lateral driving. A finite force is necessary to overcome the pinning influence even of microscale heterogeneities. The depinning dynamics of three-dimensional drops is studied for hydrophilic and hydrophobic wettability defects using a long-wave evolution equation for the film thickness profile. It is found that the nature of the depinning transition explains the experimentally observed stick-slip motion.Comment: 6 pages, 9 figures, submitted to ep

Solidification fronts in supercooled liquids: how rapid fronts can lead to disordered glassy solids

We determine the speed of a crystallisation (or more generally, a solidification) front as it advances into the uniform liquid phase after the system has been quenched into the crystalline region of the phase diagram. We calculate the front speed by assuming a dynamical density functional theory model for the system and applying a marginal stability criterion. Our results also apply to phase field crystal (PFC) models of solidification. As the solidification front advances into the unstable liquid phase, the density profile behind the advancing front develops density modulations and the wavelength of these modulations is a dynamically chosen quantity. For shallow quenches, the selected wavelength is precisely that of the crystalline phase and so well-ordered crystalline states are formed. However, when the system is deeply quenched, we find that this wavelength can be quite different from that of the crystal, so that the solidification front naturally generates disorder in the system. Significant rearrangement and ageing must subsequently occur for the system to form the regular well-ordered crystal that corresponds to the free energy minimum. Additional disorder is introduced whenever a front develops from random initial conditions. We illustrate these findings with results obtained from the PFC.Comment: 14 pages, 7 figure

Dewetting of thin films on heterogeneous substrates: Pinning vs. coarsening

We study a model for a thin liquid film dewetting from a periodic heterogeneous substrate (template). The amplitude and periodicity of a striped template heterogeneity necessary to obtain a stable periodic stripe pattern, i.e. pinning, are computed. This requires a stabilization of the longitudinal and transversal modes driving the typical coarsening dynamics during dewetting of a thin film on a homogeneous substrate. If the heterogeneity has a larger spatial period than the critical dewetting mode, weak heterogeneities are sufficient for pinning. A large region of coexistence between coarsening dynamics and pinning is found.Comment: 4 pages, 4 figure

Stability analysis of polarized domains

Polarized ferrofluids, lipid monolayers and magnetic bubbles form domains with deformable boundaries. Stability analysis of these domains depends on a family of nontrivial integrals. We present a closed form evaluation of these integrals as a combination of Legendre functions. This result allows exact and explicit formulae for stability thresholds and growth rates of individual modes. We also evaluate asymptotic behavior in several interesting limits.Comment: 12 pages, 3 figures, Late

Infants’ preference for social interactions increases from 7 to 13 months of age

This study examined 7-to-13.5-month-old middle-class Western infants’ visual orienting to third-party interactions in parallel with their social attention behavior during own social interactions (Leipzig, Germany). In Experiment 1, 9.5- to-11-month-olds (n = 20) looked longer than 7- to-8.5-month-olds (n = 20) at videos showing two adults interacting with one another when simultaneously presented with a scene showing two adults acting individually. Moreover, older infants showed higher social engagement (including joint attention) during parent–infant free play. Experiment 2 replicated this age-related increase in both measures and showed that it follows continuous trajectories from 7 to 13.5 months (n = 50). This suggests that infants’ attentional orienting to others’ interactions coincides with parallel developments in their social attention behavior during own social interactions

Liquid drops on a surface: using density functional theory to calculate the binding potential and drop profiles and comparing with results from mesoscopic modelling

The contribution to the free energy for a film of liquid of thickness $h$ on a solid surface, due to the interactions between the solid-liquid and liquid-gas interfaces is given by the binding potential, $g(h)$. The precise form of $g(h)$ determines whether or not the liquid wets the surface. Note that differentiating $g(h)$ gives the Derjaguin or disjoining pressure. We develop a microscopic density functional theory (DFT) based method for calculating $g(h)$, allowing us to relate the form of $g(h)$ to the nature of the molecular interactions in the system. We present results based on using a simple lattice gas model, to demonstrate the procedure. In order to describe the static and dynamic behaviour of non-uniform liquid films and drops on surfaces, a mesoscopic free energy based on $g(h)$ is often used. We calculate such equilibrium film height profiles and also directly calculate using DFT the corresponding density profiles for liquid drops on surfaces. Comparing quantities such as the contact angle and also the shape of the drops, we find good agreement between the two methods. We also study in detail the effect on $g(h)$ of truncating the range of the dispersion forces, both those between the fluid molecules and those between the fluid and wall. We find that truncating can have a significant effect on $g(h)$ and the associated wetting behaviour of the fluid.Comment: 16 pages, 13 fig

Quantitative assignment of reaction directionality in a multicompartmental human metabolic reconstruction.

To access publisher's full text version of this article, please click on the hyperlink in Additional Links field or click on the hyperlink at the top of the page marked Files. This article is open access.Reaction directionality is a key constraint in the modeling of genome-scale metabolic networks. We thermodynamically constrained reaction directionality in a multicompartmental genome-scale model of human metabolism, Recon 1, by calculating, in vivo, standard transformed reaction Gibbs energy as a function of compartment-specific pH, electrical potential, and ionic strength. We show that compartmental pH is an important determinant of thermodynamically determined reaction directionality. The effects of pH on transport reaction thermodynamics are only seen to their full extent when metabolites are represented as pseudoisomer groups of multiple protonated species. We accurately predict the irreversibility of 387 reactions, with detailed propagation of uncertainty in input data, and manually curate the literature to resolve conflicting directionality assignments. In at least half of all cases, a prediction of a reversible reaction directionality is due to the paucity of compartment-specific quantitative metabolomic data, with remaining cases due to uncertainty in estimation of standard reaction Gibbs energy. This study points to the pressing need for 1), quantitative metabolomic data, and 2), experimental measurement of thermochemical properties for human metabolites.Icelandic Research Fund/00406022 eu-repo/grantAgreement/EC/FP7/23281