Stratification of polymer mixtures in drying droplets: hydrodynamics and diffusion

Abstract

We study the evaporation-induced stratification of a mixture of short and long polymer chains in a drying droplet using molecular simulations. We systematically investigate the effects of hydrodynamic interactions (HI) on this process by comparing hybrid simulations accounting for HI between polymers through the multiparticle collision dynamics technique with free-draining Langevin dynamics simulations neglecting the same. We find that the dried supraparticle morphologies are homogeneous when HI are included but are stratified in core--shell structures (with the short polymers forming the shell) when HI are neglected. The simulation methodology unambiguously attributes this difference to the treatment of the solvent in the two models. We rationalize the presence (or absence) of stratification by measuring phenomenological multicomponent diffusion coefficients for the polymer mixtures. The diffusion coefficients show the importance of not only solvent backflow but also HI between polymers in controlling the dried supraparticle morphology.

arXiv comment13 pages, 9 figures

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Cited by in corpus (8)

• Diffusion and sedimentation in colloidal suspensions using multiparticle collision dynamics with a discrete particle model
• Perspective: New directions in dynamical density functional theory
• Dynamic density functional theory for drying colloidal suspensions: Comparison of hard-sphere free-energy functionals
• Modeling Solution Drying by Moving a Liquid-Vapor Interface: Method and Applications
• Exploring the role of hydrodynamic interactions in spherically-confined drying colloidal suspensions
• Transport properties of monodisperse and bidisperse hard-sphere colloidal suspensions from multiparticle collision dynamics simulations
• Inverse design of drying-induced assembly of multicomponent colloidal-particle films using surrogate models
• Effects of skewing collision cells on transport properties in multiparticle collision dynamics simulations