Reconfigurable Droplet-Droplet Communication Mediated by Photochemical Marangoni Flows

Droplets are attractive building blocks for dynamic matter that organizes into adaptive structures. Communication among collectively operating droplets opens untapped potential in settings that vary from sensing, optics, protocells, computing, or adaptive matter. Inspired by the transmission of signals among decentralized units in slime mold Physarum polycephalum, we introduce a combination of surfactants, self-assembly, and photochemistry to establish chemical signal transfer among droplets. To connect droplets that float at an air-water interface, surfactant triethylene glycol monododecylether (C₁₂E₃) is used for its ability to self-assemble into wires called myelins. We show how the trajectory of these myelins can be directed toward selected photoactive droplets upon UV exposure. To this end, we developed a strategy for photocontrolled Marangoni flow, which comprises (1) the liquid crystalline coating formed at the surface of an oleic acid/sodium oleate (OA/NaO) droplet when in contact with water, (2) a photoacid generator that protonates sodium oleate upon UV exposure and therefore disintegrates the coating, and (3) the surface tension gradient that is generated upon depletion of the surfactant from the air-water interface by the uncoated droplet. Therefore, localized UV exposure of selected OA/NaO droplets results in attraction of the myelins such that they establish reconfigurable connections that self-organize among the C₁₂E₃ and OA/NaO droplets. As an example of communication, we demonstrate how the myelins transfer fluorescent dyes, which are selectively delivered in the droplet interior upon photochemical regulation of the liquid crystalline coating.