Liquid-Liquid Phase Separation in an Elastic Network

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 tunable size can be produced through arrested phase separation in an elastic matrix. Starting with a cross-linked, 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 tunable 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 correlations between nuclei positions in determining the droplet size and polydispersity. This phenomenon has potential applications ranging from colloid synthesis and structural color to phase separation in biological cells.