Asymmetric Self‐Assembly of Colloidal Superstructures in Nested Transient Emulsion Aerosols

Abstract Emulsions are versatile and robust platforms for colloidal self‐assembly, but their ability to create complex and functional superstructures is hindered by the inherent symmetry of droplets. Here the creation of an aerosol of nested transient emulsion droplets with inherent asymmetry is reported, achieved by converging beams of water and 1‐butanol mists. Self‐assembly of nanoparticles occurs within such emulsion droplets as driven by the rapid two‐phase interface diffusion, producing anisotropic superstructures. A unique hollowing process is observed due to the asymmetric diffusion of solvents, akin to the Kirkendall effect. This novel assembly platform offers several advantages, including asymmetric self‐assembly in air, surfactant‐free operation, and tunable droplet size. It enables the creation of clean, functional nanoparticle superstructures that can be easily disassembled when needed. These advancements pave the way for exploring intricate, anisotropic superstructures with diverse applications that are unavailable in conventional superstructures of spherical symmetry.