Run-and-halt motility of droplets in response to light.

Microscopic motility is a property that emerges from systems of interacting molecules. Unraveling the mechanisms underlying such motion requires coupling the chemistry of molecules with physical processes that operate at larger length scales. Here, we show that photoactive micelles composed of molecular switches gate the autonomous motion of oil droplets in water. These micelles switch from large trans-micelles to smaller cis-micelles in response to light, and only the trans-micelles are effective fuel for the motion. Ultimately, it is this light that controls the movement of the droplets via the photochemistry of the molecules composing the micelles used as fuel. Notably, the droplets evolve positive photokinetic movement, and in patchy light environments, they preferentially move toward peripheral areas as a result of the difference in illumination conditions at the periphery. Our findings demonstrate that engineering the interplay between molecular photo-chemistry and microscopic motility allows designing motile systems rationally.

Motile behaviour of droplets in lipid systems.

Motility is the capacity for living organisms to move autonomously and with purpose, and is essential to life. The transition from abiotic chemistry into motile cellular compartments has yet to be understood, but motile behaviour likely followed chemical evolution because primeval cell survival depended on scouting for resources effectively. Minimalistic motile systems provide an experimental framework to delineate the emergence mechanisms of such an evolutionary asset. In this Review, we discuss frontier developments in controlling the movement of droplets in lipid systems, in particular, chemotactic behaviours driven by fluctuations in interfacial tension, because of its simple mechanism and prebiotic relevance. Although most efforts have focused on designing oil droplet motility in lipid-rich aqueous solutions, we highlight that water droplets can also move in lipid-enriched oils. First, we describe how droplets evolve chemotactic motility in lipid systems. Next, we review how these oil droplets can adapt their movement to illumination conditions. Finally, we discuss examples where chemical reactivity brings complexity to motility. This work contributes to systems chemistry, where chemical reactions combined with physicochemical phenomena can yield new functions, such that a limited set of molecules can promote complex movement at larger functional scales by following the rules of molecular chemistry.

Acceleration of lipid reproduction by emergence of microscopic motion.

Self-reproducing molecules abound in nature where they support growth and motion of living systems. In artificial settings, chemical reactions can also show complex kinetics of reproduction, however integrating self-reproducing molecules into larger chemical systems remains a challenge towards achieving higher order functionality. Here, we show that self-reproducing lipids can initiate, sustain and accelerate the movement of octanol droplets in water. Reciprocally, the chemotactic movement of the octanol droplets increases the rate of lipid reproduction substantially. Reciprocal coupling between bond-forming chemistry and droplet motility is thus established as an effect of the interplay between molecular-scale events (the self-reproduction of lipid molecules) and microscopic events (the chemotactic movement of the droplets). This coupling between molecular chemistry and microscopic motility offers alternative means of performing work and catalysis in micro-heterogeneous environments.