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Soft nanoparticles hold promise as smart emulsifiers due to their high degreeof deformability, permeability and stimuli responsive properties. By means oflarge-scale simulations we investigate the structural properties of nanogels atliquid-liquid (A-B) interfaces and the miscibility of the liquids inside thenanogels, covering the whole range of interfacial strength from the limit ofsingle-liquid to the case of stiff interfaces. To study the role of theinternal architecture and deformability of the nanogel we simulate a realisticdisordered and an ideal regular network, for a broad range of cross-linkingdegrees. Unlike in previous investigations on liquid miscibility, excludedvolume interactions are considered for both the monomers and the explicitsolvent particles. The nanogel permeability is analysed by using an unbiasedgrid representation that accounts for the surface fluctuations and adds to thedensity profiles the exact number of liquid particles inside the nanogel. Thebetter packing efficiency of the regular network leads to higher values of thetotal liquid uptake and the invasive capacity (A-particles in B-side andviceversa than in the disordered network, though differences vanish in thelimit of rigid interfaces. Uptake and invasion are optimized at a cross-linkingdegree that depends on the interfacial strength, tending to 15 - 20% formoderate and stiff interfaces. As the interfacial strength increases, themiscibility inside the nanogel is enhanced by a factor of up to 5 with respectto the bare interface, with the disordered networks providing a better mixingthan their ideal counterparts. The emerging scenario reported here providesgeneral guidelines for tuning the shape, uptake, invasive, and mixingcapacities of nanogels adsorbed at liquid-liquid interfaces.

Deformability and Solvent Penetration in Soft Nanoparticles at Liquid-Liquid Interfaces