Photoswitchable Dissipative Two‐Dimensional Colloidal Crystals

Control over particle interactions and organization at fluid interfaces is of great importance both for fundamental studies and practical applications. Rendering these systems stimulus-responsive is thus a desired challenge both for investigating dynamic phenomena and realizing reconfigurable materials. Here, we describe the first reversible photocontrol of two-dimensional colloidal crystallization at the air/water interface, where millimeter-sized assemblies of microparticles can be actuated through the dynamic adsorption/desorption behavior of a photosensitive surfactant added to the suspension. This allows us to dynamically switch the particle organization between a highly crystalline (under light) and a disordered (in the dark) phase with a fast response time (crystallization in approximate to 10 s, disassembly in approximate to 1 min). These results evidence a new kind of dissipative system where the crystalline state can be maintained only upon energy supply.