Branching out and back: Reconfigurable nematic drops driven by molecular heterogeneity*

Traditionally, polydispersity in matter is often avoided, since it tends to impede self-assembly and state transformation. Here we report reconfigurable nematic liquid crystal oligomer drops, which reveal, surprisingly, that molecular heterogeneity facilitates equilibrium transitions among dramatically different morphological structures, via spatial segregation. Specifically, fine-tuning the temperature and oligomer chain length distribution alters the balance between interfacial tension and liquid crystal elasticity, driving spontaneous formation of roughened spheres, flowers, and highly branched filamentous networks with uniform and controllable diameters. This feature provides potential connections to surface patterning in biological world, such as pollen grains. Further, we employ the achieved structures to template assembly of plasmonic nanoparticles, as well as helical coils with chiral dopant. With the capabilities of being produced reversibly and permanently locked into liquid crystal elastomers, the demonstrated simple rules thus offer new routes for programmed spatio-temporal networks.