Self-Organized Antipodal Multifunctional Micromotors via Evaporative Liquid-Liquid Phase Separation

Abstract

Active microparticles with spatially organized multifunctionality could enable new forms of autonomous transport and chemical activity, yet creating such architectures within individual particles remains challenging. Here, we show that such complex functional architectures emerge spontaneously when multiple functional components (enzymes, nanoparticles, etc.) are introduced into evaporating multicomponent droplets undergoing liquid-liquid phase separation. Coupled Marangoni flows and interfacial dynamics drive the asymmetric localization of functional nanoparticles, positioning distinct functionalities on opposite sides of a microparticle in an architecture we term antipodal. This organization generates emergent magnetic anisotropy when magnetic nanoparticles are incorporated, enabling catalytically propelled motion parallel or antiparallel to a uniform magnetic field without an external chemical gradient. We also demonstrate enzyme-enzyme antipodal micromotors that combine weak chemotactic steering with strong propulsion driven by a spatially uniform chemical fuel, a strategy relevant to environments where chemical gradients are weak. Extensive theoretical modelling elucidates the underlying interplay of Marangoni flows and interfacial dynamics, providing a mechanistic basis for tunability. Our findings establish a route to spatially programmed active matter, in which functional architectures and directional capabilities emerge spontaneously through coupled hydrodynamic and interfacial dynamics.