Phase separation effects on a partially miscible viscous fingering dynamics

Classical viscous fingering (VF) instability, the formation of finger-like interfacial patterns, occurs when a less viscous fluid displaces a more viscous one in porous media in immiscible and fully miscible systems. However, the dynamics in partially miscible fluid pairs, exhibiting a phase separation due to its finite solubility into each other, has not been largely understood so far. This study has succeeded in experimentally changing the solution system from immiscible to fully miscible or partially miscible by varying the compositions of the components in an aqueous two-phase system (ATPS) while leaving the viscosities relatively unchanged at room temperature and atmospheric pressure. Here, we have experimentally discovered a new topological transition of VF instability by performing a Hele-Shaw cell experiment using the partially miscible system. The finger formation in the investigated partially miscible system changes to the generation of spontaneously moving multiple droplets. Through additional experimental investigations, we determine that such anomalous VF dynamics is driven by thermodynamic instability such as phase separation due to spinodal decomposition and Korteweg convection induced by compositional gradient during such phase separation. We perform the numerical simulation by coupling hydrodynamics with such chemical thermodynamics and the spontaneously moving droplet dynamics is obtained, which is in good agreement with the experimental investigations of the ATPS. This numerical result strongly supports our claim that the origin of such anomalous VF dynamics is thermodynamic instability.