Our group has demonstrated that emulsions functionalized with DNA strands on their surface self-assemble into clusters whose architecture is governed by the number and size of adhesion patches that form between droplets. The hybridization of single stranded linkers drives the formation of these adhesive domains, which are enriched in mobile binders. This work established a general principle: mobile binders convert molecular-scale interactions into programmable, equilibrium valence at the colloidal scale. The framework applies broadly to droplets, vesicles, lipid-coated solids, and even biological cells.
We derive and experimentally test an equilibrium theory that captures the adhesion of DNA-coated emulsion droplets. Notably, we identify a transition from spherical to deformed droplet binding at a characteristic DNA coverage that depends on molecular properties and surface tension.
We report the first realization of oil microdroplets that are simultaneously density- and refractive-index matched with a biocompatible aqueous phase, providing full optical access to the three-dimensional structure of programmable DNA-mediated droplet assemblies.
We demonstrate how mobile DNA linkers self-organize at the interface between colloidal droplets into a well-defined number of adhesive patches, that is, valence, to create order on much longer length scales. We demonstrate that this valence is a thermodynamic equilibrium state, which is tuned by the number and sequence of DNAs, and the patch geometry.
Grafting DNA onto liquid interfaces of emulsions leads to exciting new architectural possibilities due to the mobility of the DNA ligands and the patches they form between bound droplets. Here we show that the size and number of these adhesion patches (valency) can be controlled. Valence 2 leads to flexible polymers of emulsion droplets, while valence above 4 leads to rigid droplet networks.