Higher-order structures that originate from the specific and re- versible DNA-directed self-assembly of microscopic building blocks hold great promise for future technologies. Here, we functional- ized biotinylated soft colloid oil-in-water emulsion droplets with biotinylated single-stranded DNA oligonucleotides using strepta- vidin as an intermediary linker. We show the components of this modular linking system to be stable and to induce sequence- specific aggregation of binary mixtures of emulsion droplets. Three length scales were thereby involved: nanoscale DNA base pairing linking microscopic building blocks resulted in macroscopic aggre- gates visible to the naked eye. The aggregation process was reversible by changing the temperature and electrolyte concentra- tion and by the addition of competing oligonucleotides. The system was reset and reused by subsequent refunctionalization of the emulsion droplets. DNA-directed self-assembly of oil-in-water emulsion droplets, therefore, offers a solid basis for programmable and recyclable soft materials that undergo structural rearrange- ments on demand and that range in application from information technology to medicine.
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