Abstract
Living and engineered systems rely on the stable coexistence of two interspersed liquid phases. Yet surface tension drives their complete separation. Here we show that stable droplets of uniform and tuneable size can be produced through arrested phase separation in an elastic matrix. Starting with an elastic polymer network swollen by a solvent mixture, we change the temperature or composition to drive demixing. Droplets nucleate and grow to a stable size that is tuneable by the network cross-linking density, the cooling rate, and the composition of the solvent mixture. We discuss thermodynamic and mechanical constraints on the process. In particular, we show that the threshold for macroscopic phase separation is altered by the elasticity of the polymer network, and we highlight the role of internuclear correlations in determining the droplet size and polydispersity. This phenomenon has potential applications ranging from colloid synthesis and structural colour to phase separation in biological cells.
Highlights
Nucleation and growth of liquid droplets is a ubiquitous process
We demonstrate its efficacy for both temperature- and composition-driven condensation inside of covalently or physically cross-linked polymer networks swollen with silicone or aqueous solvents
The interaction of condensation and network elasticity may play a role in the cellular physiology of phase-separated proteins, and the physical parameters identified here could possibly be exploited by living cells to regulate phase separation [16,21]
Summary
Nucleation and growth of liquid droplets is a ubiquitous process. In the sky above us, it underlies the formation of clouds. We investigate nucleation and growth of liquid droplets inside of a cross-linked polymer network. We demonstrate its efficacy for both temperature- and composition-driven condensation inside of covalently or physically cross-linked polymer networks swollen with silicone or aqueous solvents. This process may provide a flexible route to the bulk synthesis of monodisperse, polymeric microparticles and nanoparticles and enable the self-assembly of flexible, structurally colored materials [19,20]. The interaction of condensation and network elasticity may play a role in the cellular physiology of phase-separated proteins, and the physical parameters identified here could possibly be exploited by living cells to regulate phase separation [16,21]
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