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We demonstrate the dynamic control of aqueous two phase system (ATPS) droplets in shrinking, growing, and dissolving conditions. The ATPS droplets are formed passively in a flow focusing microfluidic channel, where the dextran-rich (DEX) and polyethylene glycol-rich (PEG) solutions are introduced as disperse and continuous phases, respectively. To vary the ATPS equilibrium condition, we infuse into a secondary inlet the PEG phase from a different polymer concentration ATPS. We find that the resulting alteration of the continuous PEG phase can cause droplets to shrink or grow by approximately 45 and 30%, respectively. This volume change is due to water exchange between the disperse DEX and continuous PEG phases, as the system tends towards new equilibria. We also develop a simple model, based on the ATPS binodal curve and tie lines, that predicts the amount of droplet shrinkage or growth, based on the change in the continuous phase PEG concentration. We observe a good agreement between our experimental results and the model. Additionally, we find that when the continuous phase PEG concentration is reduced such that PEG and DEX phases no longer phase separate, the ATPS droplets are dissolved into the continuous phase. We apply this method to controllably release encapsulated microparticles and cells, and we find that their release occurs within 10 seconds. Our approach uses the dynamic equilibrium of ATPS to control droplet size along the microfluidic channel. By modulating the ATPS equilibrium, we are able to shrink, grow, and dissolve ATPS droplets in situ. We anticipate that this approach may find utility in many biomedical settings, for example, in drug and cell delivery and release applications.

Shrinking, growing, and bursting: microfluidic equilibrium control of water-in-water droplets