Controlled evaporation-induced phase separation of droplets containing nanogels and salt molecules

Droplets without protection from surfactants or surfactant-like objects normally experience merging or a coalescence process since it is thermodynamically favored. However, division or replication of droplets is thermodynamically unfavored and comparably more difficult to realize. Herein, we demonstrate that a population of droplets that are composed of nanogels and salt spontaneously undergo a separation process under a slow solvent evaporation condition. Each individual droplet underwent changes in size, shape and eventually developed into two domains, which was caused by the screening effect due to the increased salt concentration as a result of solvent evaporation. The two domains gradually separated into nanogel-rich and salt-rich parts. These two parts eventually evolved into nanogel aggregates and branched structures, respectively. This separation was mainly due to the salting out effect and dewetting. Comparison studies indicate that both the nanogels and salt are indispensable ingredients for the phase separation. These discoveries may have profound applications in the fields of biomimetics and offer new routes for self-replication systems.