Light-driven active phase separation and droplet division

Abstract

Phase separation organizes matter across scales, yet how it operates under sustained energy input remains poorly understood. Experimental approaches to driven phase separation have largely relied on chemically fueled systems, in which reaction fluxes are intrinsically coupled to fuel consumption and reaction-network complexity. Here we show that continuous molecular switching alone is sufficient to generate active phase behavior in a minimal two-phase system. Using light-responsive DNA-azobenzene coacervates confined in microfluidic droplets, we modulate intermolecular interactions with spatiotemporal precision and quantitatively track phase separation dynamics under illumination. Light-driven azobenzene isomerization controls both thermodynamics and kinetics, setting phase boundaries and regulating dissolution and nucleation rates. Under single-wavelength illumination that couples forward and backward isomerization into a dynamic photostationary state, coarsening is arrested and micron-sized coacervates are stabilized. When the two photoisomerization pathways are driven independently, spatially unbalanced reaction fluxes generate sustained interfacial instabilities, including surface undulations, budding, and division. These behaviors arise from a physical coupling between reaction kinetics and phase separation, without chemical fuels or biochemical regulation. Our results show that non-equilibrium phase behavior is governed by how opposing reaction fluxes are imposed, establishing reversible molecular switching as a minimal route to active materials from equilibrium building blocks.