Modeling Evaporation and Particle Assembly in Colloidal Droplets.

Evaporation-induced assembly of nanoparticles in a drying droplet is of great importance in many engineering applications, including printing, coating, and thin film processing. The investigation of particle dynamics in evaporating droplets can provide fundamental hydrodynamic insight for revealing the processing-structure relationship in the particle self-organization induced by solvent evaporation. We develop a free-energy-based multiphase lattice Boltzmann method coupled with Brownian dynamics to simulate evaporating colloidal droplets on solid substrates with specified wetting properties. The influence of interface-bound nanoparticles on the surface tension and evaporation of a flat liquid-vapor interface is first quantified. The results indicate that the particles at the interface reduce surface tension and enhance evaporation flux. For evaporating particle-covered droplets on substrates with different wetting properties, we characterize the increase of evaporate rate via measuring droplet volume. We find that droplet evaporation is determined by the number density and circumferential distribution of interfacial particles. We further correlate particle dynamics and assembly to the evaporation-induced convection in the bulk and on the surface of droplet. Finally, we observe distinct final deposits from evaporating colloidal droplets with bulk-dispersed and interface-bound particles. In addition, the deposit pattern is also influenced by the equilibrium contact angle of droplet.