We report on the effect of intermolecular forces on the fluctuations of supported liquid films. Using an optically-induced thermal gradient, we form nanometer-thin films of wetting liquids on glass substrates, where van der Waals forces are balanced by thermocapillary forces. We show that the fluctuation dynamics of the film interface is strongly modified by intermolecular forces at lower frequencies. Data spanning three frequency decades are in excellent agreement with theoretical predictions accounting for van der Waals forces. Our results emphasize the relevance of intermolecular forces on thermal fluctuations when fluids are confined at the nanoscale.
Within mean-field theory we study wetting of elastic substrates. Our analysis is based on a grand canonical free energy functional of the fluid number density and of the substrate displacement field. The substrate is described in terms of the linear theory of elasticity, parametrized by two Lame coefficients. The fluid contribution is of the van der Waals type. Two potentials characterize the interparticle interactions in the system. The long-ranged attraction between the fluid particles is described by a potential $w(r)$, and $v(r)$ characterizes the substrate-fluid interaction. By integrating out the elastic degrees of freedom we obtain an effective theory for the fluid number density alone. Its structure is similar to the one for wetting of an inert substrate. However, the potential $w(r)$ is replaced by an effective potential which, in addition to $w(r)$, contains a term bilinear in $v(r)$. We discuss the corresponding wetting transitions in terms of an effective interface potential $omega(ell)$, where $ell$ denotes the thickness of the wetting layer. We show that in the case of algebraically decaying interactions the elasticity of the substrate may suppress critical wetting transitions, and may even turn them first order.
Driving an inertial many-body system out of equilibrium generates complex dynamics due to memory effects and the intricate relationships between the external driving force, internal forces, and transport effects. Understanding the underlying physics is challenging and often requires carrying out case-by-case analysis. To systematically study the interplay between all types of forces that contribute to the dynamics, a method to generate prescribed flow patterns could be of great help. We develop a custom flow method to numerically construct the external force field required to obtain the desired time evolution of an inertial many-body system, as prescribed by its one-body current and density profiles. We validate the custom flow method in a Newtonian system of purely repulsive particles by creating a slow motion dynamics of an out-of-equilibrium process and by prescribing the full time evolution between two distinct equilibrium states. The method can also be used with thermostat algorithms to control the temperature.
We describe a series of experiments and computer simulations on vibrated granular media in a geometry chosen to eliminate gravitationally induced settling. The system consists of a collection of identical spherical particles on a horizontal plate vibrating vertically, with or without a confining lid. Previously reported results are reviewed, including the observation of homogeneous, disordered liquid-like states, an instability to a `collapse of motionless spheres on a perfect hexagonal lattice, and a fluctuating, hexagonally ordered state. In the presence of a confining lid we see a variety of solid phases at high densities and relatively high vibration amplitudes, several of which are reported for the first time in this article. The phase behavior of the system is closely related to that observed in confined hard-sphere colloidal suspensions in equilibrium, but with modifications due to the effects of the forcing and dissipation. We also review measurements of velocity distributions, which range from Maxwellian to strongly non-Maxwellian depending on the experimental parameter values. We describe measurements of spatial velocity correlations that show a clear dependence on the mechanism of energy injection. We also report new measurements of the velocity autocorrelation function in the granular layer and show that increased inelasticity leads to enhanced particle self-diffusion.
When an external field drives a colloidal system out of equilibrium, the ensuing colloidal response can be very complex and obtaining a detailed physical understanding often requires case-by-case considerations. In order to facilitate systematic analysis, here we present a general iterative scheme for the determination of the unique external force field that yields a prescribed inhomogeneous stationary or time-dependent flow in an overdamped Brownian many-body system. The computer simulation method is based on the exact one-body force balance equation and allows to specifically tailor both gradient and rotational velocity contributions, as well as to freely control the one-body density distribution. Hence compressibility of the flow field can be fully adjusted. The practical convergence to a unique external force field demonstrates the existence of a functional map from both velocity and density to external force field, as predicted by the power functional variational framework. In equilibrium, the method allows to find the conservative force field that generates a prescribed target density profile, and hence implements the Mermin-Evans classical density functional map from density distribution to external potential. The conceptual tools developed here enable one to gain detailed physical insight into complex flow behaviour, as we demonstrate in prototypical situations.
The rheology of pressure-driven flows of two-dimensional dense monodisperse emulsions in neutral wetting microchannels is investigated by means of mesoscopic lattice simulations, capable of handling large collections of droplets, in the order of several hundreds. The simulations reveal that the fluidization of the emulsion proceeds through a sequence of discrete steps, characterized by yielding events whereby layers of droplets start rolling over each other, thus leading to sudden drops of the relative effective viscosity. It is shown that such discrete fluidization is robust against loss of confinement, namely it persists also in the regime of small ratios of the droplet diameter over the microchannel width. We also develop a simple phenomenological model which predicts a linear relation between the relative effective viscosity of the emulsion and the product of the confinement parameter (global size of the device over droplet radius) and the viscosity ratio between the disperse and continuous phases. The model shows excellent agreement with the numerical simulations. The present work offers new insights to enable the design of microfluidic scaffolds for tissue engineering applications and paves the way to detailed rheological studies of soft-glassy materials in complex geometries.