Coacervate micro-droplets produced by liquid-liquid phase separation are increasingly used to emulate the dynamical organization of membraneless organelles found in living cells. Designing synthetic coacervates able to be formed and disassembled with improved spatiotemporal control is still challenging. In this chapter, we describe the design of photoswitchable coacervate droplets produced by phase separation of short double stranded DNA in the presence of an azobenzene cation. The droplets can be reversibly dissolved with light, which provides a new approach for the spatiotemporal regulation of coacervation. Significantly, the dynamics of light-actuated droplet formation and dissolution correlates with the capture and release of guest solutes. The reported system can find applications for the dynamic photocontrol of biomolecule compartmentalization, paving the way to the light-activated regulation of signaling pathways in artificial membraneless organelles.

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