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We report observations of the self-assembly of coated droplets into regular clusters at the sudden expansion of a microfluidic channel. A double emulsion consisting of a regular train of coated microdroplets was created upstream of the channel expansion, so that the inter-drop distance, droplet length, velocity and coating thickness could be varied by imposing different inlet pressures, albeit not independently. Provided that the enlarged channel remains sufficiently confined to prohibit propagation in double file, droplets can assemble sequentially into regular linear clusters at the expansion. Droplets join a cluster via the coalescence of their coating film with that of the group ahead. This coalescence occurs when the droplets approach each other to within a critical distance at the expansion, enabled by hydrodynamic interactions within the train. Clusters comprising a finite number of droplets are obtained because reconfiguration of the droplet assembly during coalescence increases the distance to the following droplet. Decreasing the inter-drop distance increases the cluster size up to a maximum value beyond which continuous clusters form. Formalising these observations in a simple model reveals that clusters of any size are possible but that they occur for increasingly narrow ranges of parameter values. Our experimental observations suggests that background experimental fluctuations limit the maximum discrete cluster size in practice. This method of self-assembly offers a robust alternative to flow focusing for encapsulating multiple cores in a single coating film and the potential to build more complex colloidal building blocks by de-confining the clusters.

Self-assembly of coated microdroplets at the sudden expansion of a microchannel