Self-Organization of Structured Fluids into Condensate Networks

Self-organization through liquid–liquid crystalline phase separation (LLCPS) is the process by which liquids demixing results in the formation of a solute-poor isotropic phase and a solute-rich phase exhibiting liquid-crystalline order. The liquid crystalline order of this solute-rich structured fluid can lead to the formation of non-spherical condensates. Here, I present LLCPS in smectic systems, where cooling a homogeneous mixture of a smectogenic solute and a solvent induces phase separation into condensates with diverse morphologies, including filaments, helical coils, and bulged discs. These condensates assemble into interconnected networks that display out-of-equilibrium dynamics characterized by continuous reorganization. I show how the interplay between anisotropic elasticity, interfacial tension, and hydrodynamics governs the formation of specific network topologies. Furthermore, I discuss how liquid-crystal energetics alter coarsening dynamics and can even arrest phase separation. Finally, I demonstrate strategies to control LLCPS, guiding the emergence of condensate networks with tunable porosity. This work elucidates condensate network dynamics and may open new avenues for designing fluids with life-like structures.