Self‐Organizing Microdroplet Protocells Displaying Light‐Driven Oscillatory and Morphological Evolution

Abstract The development of synthetic systems that enable the sustained active self‐assembly of molecular blocks to mimic the complexity and dynamic behavior of living systems is of great interest in elucidating the origins of life, understanding the basic principles behind biological organization, and designing active materials. However, it remains a challenge to construct microsystems with dynamic behaviors and functions that are connected to molecular self‐assembly processes driven by external energy. Here, an active self‐assembly of microdroplet protocells with dynamic structure and high structural complexity through living radical polymerization under constant energy flux is reported. The active microdroplet protocells exhibit nonlinear behaviors including oscillatory growth and shrinkage. This relies on the transient stabilization of molecular assembly, which can channel the inflow of energy through noncovalent interactions of pure synthetic components. The intercommunication of microdroplet protocells through stochastic fusion leads to the formation of a variety of dynamic and higher‐order biomimetic microstructures. This work constitutes an important step toward the realization of autonomous and dynamic microsystems and active materials with life‐like properties.