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A major theme of our research concerns the self-assembly of droplets into programmable structures, using mobile DNA binders to encode interactions, droplet valence, and large-scale geometry. Emulsion droplets provide a unique platform for this problem: unlike solid colloids, their fluid interfaces allow binders to diffuse, reorganize, and equilibrate. This mobility fundamentally alters the physics of self-assembly, enabling droplets to select their valence thermodynamically rather than having it imposed geometrically. We have shown that mobile binders allow droplets to autonomously select valence, assemble into polymers, and fold into complex architectures. Beyond materials design, this framework provides a toy model for protein folding. Our current and future research focuses on extending these ideas to 3D folds and bio-inspired materials whose function emerges from programmable, self-organized interactions.
We introduce a minimal model system of colloidal droplet chains, with programmable DNA interactions that guide their downhill folding into specific geometries. Combining experiments, simulations and theory, we show that controlling the order in which interactions are switched on directs folding into unique structures, which we call colloidal foldamers.
McMullen, Muñoz Basagoiti, et al., Self-assembly of emulsion droplets through programmable folding, Nature 610, 2022.
We control the valence of DNA-functionalized emulsions to make linear and branched model polymers, or “colloidomers.” The distribution of cluster sizes is consistent with a polymerization process in which the droplets achieve their prescribed valence. Conformational statistics reveal that the chains are freely jointed, so that the Kuhn length is close to one bead diameter.
McMullen, et al., Freely Jointed Polymers Made of Droplets, Phys. Rev. Lett. 121, 2018.
We demonstrate programmed sequential self-assembly of DNA functionalized emulsions. The droplets are initially inert because the grafted DNA strands are pre-hybridized in pairs. Active strands on initiator droplets then displace one of the paired strands and thus release its complement, which in turn activates the next droplet in the sequence, akin to living polymerization.
Zhang, et al., Sequential self-assembly of DNA functionalized droplets, Nature Comm. 8, 2017.
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