To control the spatial placement and organize micro/nanodroplets (NDs) has fundamental importance both in science and engineering. Cholesteric liquid crystal (CLC) droplets with topological diversity can offer many self-assembly modalities to arrange guest NDs in their spherical confinement; however, limited progress has been achieved due to difficulties of loading NDs into stabilized host droplets. Here, a laser injection technique is introduced, through which a controlled number of NDs were injected from a pre-selected location onto the surface of the host droplet. The sequentially injected NDs spontaneously drifted toward areas with topological defects and self-assembled along its geometry or local director field into a predefined shape. Within CLC droplets with different topological structures, guest NDs self-assembled near areas with defect points as twisting radial chains and quill-like assembly structures, and along defect lines as discrete beads and helical threads, respectively. The injection speed of the NDs, controlled by laser power, was found to play a key role in the assembly geometry of NDs as well as the internal structure of the CLC droplet processed. This study expands our abilities to precisely organize NDs in a spherical confinement and such droplet-based microsystems have potential applications for sensors, photonic devices, pharmaceuticals, and biotechnology.
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