Self‐Propelled Supracolloidal Fibers from Multifunctional Polymer Surfactants and Droplets

Advanced synthetic materials are needed to produce nano‐ and mesoscale structures that function autonomously, catalyze reactions, and convert chemical energy into motion. This paper describes supracolloidal fiber‐like structures that are composed of self‐adhering, or “sticky,” oil‐in‐water emulsion droplets. Polymer zwitterion surfactants serve as the key interfacial components of these materials, enabling multiple functions simultaneously, including acting as droplet‐stabilizing surfactants, interdroplet adhesives, and building blocks of the fibers. This fiber motion, a surprising additional feature of these supracolloidal structures, is observed at the air–water interface and hinged on the chemistry of the polymer surfactant. The origin of this motion is hypothesized to involve transport of polymer from the oil–water interface to the air–water interface, which generates a Marangoni (interfacial) stress. Harnessing this fiber motion with functional polymer surfactants, and selection of the oil phase, produced worm‐like objects capable of rotation, oscillation, and/or response to external fields. Overall, these supracolloidal fibers fill a design gap between self‐propelled nano/microscale particles and macroscale motors, and have the potential to serve as new components of soft, responsive materials structures. Supracolloidal fibers, composed of adhesive emulsion droplets, exhibit self‐driven motion at fluid interfaces. The fibers “swim” on the surface of water (air–water interface) and rotate rapidly when composed of distinct segments of connected droplets that encapsulate dense (pink) and light (white) fluids. The chemistry and interfacial activity of designer polymer zwitterionic surfactants are key drivers of these novel macroscopic fibers.