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Motile droplets using Marangoni convection are attracting attention for theirpotential as cell-mimicking small robots. However, the motion of dropletsrelative to the internal and external environments that generate Marangoniconvection has not been quantitatively described. This study used an aqueoustwo-phase system (polyethylene glycol (PEG) and dextran) in an elongatedchamber to generate motile dextran droplets in a constant PEG concentrationgradient. We demonstrated that dextran droplets move by Marangoni convection,resulting from the PEG concentration gradient and the active transport of PEGand dextran into and out of the droplet. Furthermore, by spontaneouslyincorporating long DNA into the dextran droplets, we achieved cell-likemotility changes controlled by coexisting environment-sensing molecules. TheDNA changes its position within the droplet and motile speed in response toexternal conditions. In the presence of Mg2+, the coil-globule transition ofDNA inside the droplet accelerates the motile speed due to the decrease in thedroplet's dynamic viscosity. Globule DNA condenses at the rear part of thedroplet along the convection, while coil DNA moves away from the droplet'scentral axis, separating the dipole convections. These results provide ablueprint for designing autonomous small robots using phase-separated droplets,which change the mobility and molecular distribution within the droplet inreaction to the environment. It will also open unexplored areas ofself-assembly mechanisms through phase separation under convections, such asintracellular phase separation.

Marangoni droplets of dextran in PEG solution and its motile change due to coil-globule transition of coexisting DNA