Circulating Marangoni flows within droplets in smectic films.

We present a theoretical study and numerical simulation of Marangoni convection within ellipsoidal isotropic droplets embedded in free-standing smectic films (FSSFs). The thermocapillary flows are analyzed for both isotropic droplets spontaneously formed in FSSF overheated above the bulk smectic-isotropic transition and oil lenses deposited on the surface of the smectic film. The realistic model for which the upper drop interface is free from the smectic layers, while at the lower drop surface the smectic layering persists is considered in detail. For isotropic droplets and oil lenses this leads effectively to a sticking of fluid motion at the border with a smectic shell. The above mentioned asymmetric configuration is realized experimentally when the temperature of the upper side of the film is higher than at the lower one. The full set of stationary solutions for Stokes stream functions describing the Marangoni convection flows within the ellipsoidal drops are derived analytically. The temperature distribution in the ellipsoidal drop and the surrounding air is determined in the frame of the perturbation theory. As a result, the analytical solutions for the stationary thermocapillary convection are obtained for different droplet ellipticity ratios and the heat conductivity of the liquid crystal and air. In parallel, the numerical hydrodynamic calculations of the thermocapillary motion in drops are made. Both analytical and numerical simulations predict the axially symmetric circulatory convection motion determined by the Marangoni effect at the droplet-free surface. Due to a curvature of the drop interface a temperature gradient along its free surface always exists. Thus, the thermocapillary convection within the ellipsoidal droplets in overheated FSSF is possible for the arbitrarily small Marangoni numbers. Possible experimental observations enabling the checking of our predictions are proposed.

Applying droplets and films in evaporative lithography.

This review covers experimental results of evaporative lithography and analyzes existing mathematical models of this method. Evaporating droplets and films are used in different fields, such as cooling of heated surfaces of electronic devices, diagnostics in health care, creation of transparent conductive coatings on flexible substrates, and surface patterning. A method called evaporative lithography emerged after the connection between the coffee ring effect taking place in drying colloidal droplets and naturally occurring inhomogeneous vapor flux densities from liquid-vapor interfaces was established. Essential control of the colloidal particle deposit patterns is achieved in this method by producing ambient conditions that induce a nonuniform evaporation profile from the colloidal liquid surface. Evaporative lithography is part of a wider field known as "evaporative-induced self-assembly" (EISA). EISA involves methods based on contact line processes, methods employing particle interaction effects, and evaporative lithography. As a rule, evaporative lithography is a flexible and single-stage process with such advantages as simplicity, low price, and the possibility of application to almost any substrate without pretreatment. Since there is no mechanical impact on the template in evaporative lithography, the template integrity is preserved in the process. The method is also useful for creating materials with localized functions, such as slipperiness and self-healing. For these reasons, evaporative lithography attracts increasing attention and has a number of noticeable achievements at present. We also analyze limitations of the approach and ways of its further development.

Joint effect of advection, diffusion, and capillary attraction on the spatial structure of particle depositions from evaporating droplets.

A simplified model is developed, which allows us to perform computer simulations of the particles transport in an evaporating droplet with a contact line pinned to a hydrophilic substrate. The model accounts for advection in the droplet, diffusion, and particle attraction by capillary forces. On the basis of the simulations, we analyze the physical mechanisms of forming of individual chains of particles inside the annular sediment. The parameters chosen correspond to the experiments of Park and Moon [Langmuir 22, 3506 (2006)LANGD50743-746310.1021/la053450j], where an annular deposition and snakelike chains of colloid particles have been identified. The annular sediment is formed by advection and diffusion transport. We find that the close packing of the particles in the sediment is possible if the evaporation time exceeds the characteristic time of diffusion-based ordering. We show that the chains are formed by the end of the evaporation process due to capillary attraction of particles in the region bounded by a fixing radius, where the local droplet height is comparable to the particle size. At the beginning of the evaporation, the annular deposition is shown to expand faster than the fixing radius moves. However, by the end of the process, the fixing radius rapidly outreaches the expanding inner front of the ring. The snakelike chains are formed at this final stage when the fixing radius moves toward the symmetry axis.