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In this work, we unravel the role of surface properties of colloidalparticles on the formation of supraparticles (clusters of colloidal particles)in a colloidal Ouzo droplet. Self-lubricating colloidal Ouzo droplets are anefficient and simple approach to form supraparticles, overcoming the challengeof the coffee stain effect in situ. Supraparticles are an efficient route tohigh-performance materials in various fields, from catalysis to carriers fortherapeutics. Yet, the role of the surface of colloidal particles in theformation of supraparticles using Ouzo droplets remains unknown. Therefore, weused silica particles as a model system and compared sterically stabilizedversus electrostatically stabilized silica particles - positively andnegatively charged. Additionally, we studied the effect of hydration. Hydratednegatively charged silica particles and sterically stabilized silica particlesform supraparticles. Conversely, dehydrated negatively charged silica particlesand positively charged amine-coated particles form flat film-like deposits.Notably, the assembly process is different for all the four types of particles.The surface modifications alter (a) the contact line motion of the Ouzo dropletand (b) the particle-oil and particle-substrate interactions. These alterationsmodify the particle accumulation at the various interfaces, which ultimatelydetermines the shape of the final deposit. Thus, by modulating the surfaceproperties of the colloidal particles, we can tune the shape of the finaldeposit, from a spheroidal supraparticle to a flat deposit. In the future, thisapproach can be used to tailor the supraparticles for applications such asoptics and catalysis, where the shape affects the functionality.

Surface Properties of Colloidal Particles Affect Colloidal Self-Assembly in Evaporating Self-Lubricating Ternary Droplets