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Phase segregation triggered by selective evaporation can emerge inmulticomponent systems, leading to complex physiochemical hydrodynamics.Recently, Li et al. (Phys. Rev. Lett., vol. 120, 2018, 224501) and Kim & Stone(J. Fluid Mech., vol. 850, 2018, pp. 769-783) reported a segregative behavior(i.e., demixing) in an evaporating binary droplet. In this work, by means ofexperiments and theoretical analysis, we investigate the flow dynamics afterthe occurrence of the phase segregation. As example, we take the1,2-hexanediol-water binary droplet system. First, we experimentally reveal theoverall physiochemical hydrodynamics of the evaporation process, including thesegregative behavior and the resulting flow structure close to the substrate.By quantifying the evolution of the radial flow, we identify three successivelife stages of the evaporation process. At Stage I, a radially outward flow isobserved. It is driven by the Marangoni effect. At the transition to Stage II,the radial flow partially reverses, starting from the contact line. This flowbreaks the axial symmetry and remarkably is driven by the segregation itself.Finally at Stage III, the flow decays as the evaporation gradually ceases. Atthis stage the segregation has grown to the entire droplet, and the flow isagain controlled by the Marangoni effect. The resulting Marangoni flowhomogenizes the distribution of the entrapped volatile water over the wholedroplet.

Physiochemical hydrodynamics of the phase segregation in an evaporating binary microdroplet