There are many new approaches to designing complex anisotropic colloids, often using droplets as templates. However, droplets themselves can be designed to form anisotropic shapes without any external templates. One approach is to arrest binary droplet coalescence at an intermediate stage before a spherical shape is formed. Further shape relaxation of such anisotropic, arrested structures is retarded by droplet elasticity, either interfacial or internal. In this article we study coalescence of structured droplets, containing a network of anisotropic colloids, whose internal elasticity provides a resistance to full shape relaxation and interfacial energy minimization during coalescence. Precise tuning of droplet elasticity arrests coalescence at different stages and leads to various anisotropic shapes, ranging from doublets to ellipsoids. A simple model balancing interfacial and elastic energy is used to explain experimentally observed coalescence arrest in viscoelastic droplets. During coalescence of structured droplets the interfacial energy is continuously reduced while the elastic energy is increased by compression of the internal structure and, when the two processes balance one another, coalescence is arrested. Experimentally we observe that if either interfacial energy or elasticity dominates, total coalescence or total stability of droplets results. The stabilization mechanism is directly analogous to that in a Pickering emulsion, though here the resistance to coalescence is provided via an internal volume-based, rather than surface, structure. This study provides guidelines for designing anisotropic droplets by arrested coalescence but also explains some observations of "partial" coalescence observed in commercial foods like ice cream and whipped cream.

When two emulsion drops begin to coalesce, their complete fusion into a single spherical drop can sometimes be arrested in an intermediate shape if a rheological resistance offsets the Laplace pressure driving force. Arrested coalescence of droplets is important, both for its broad impact on commercial food production as well as its potential for fabricating novel anisotropic colloidal microstructures. We use a micromanipulation technique to demonstrate the dynamics of arrested coalescence between droplets with interfacially adsorbed colloids. Surface coverage of the droplets is precisely determined by a capillary aspiration technique and then their coalescence is studied in situ. Depending on their surface coverage, droplets can experience total coalescence, arrested coalescence or total stability. We use microscopic observations along with geometrical packing arguments to confirm that coalescence is arrested due to close-packed jamming of particles. The anisotropic Laplace stress within the arrested structure is balanced by the elastic modulus of the jammed interface and thus further relaxation of the arrested structure is halted. Precise mapping of the arrested coalescence regime at a microscopic scale helps us to anticipate its effects on bulk scale production of such anisotropic colloidal structures.

Fragrances are amphiphilic and highly volatile, all of which makes them a challenging cargo to efficiently encapsulate and retain in microcapsules using traditional approaches. We address these limitations by introducing a new strategy that combines bulk and microfluidic emulsification: a stable fragrance-in-water (F/W) emulsion that is primarily prepared from bulk emulsification is incorporated within a polymer microcapsule via microfluidic emulsification. On the basis of the in-depth study of physicochemical properties of the microcapsules on fragrance leakage, we demonstrate that enhanced retention of fragrance can be achieved by using a polar polymeric shell and forming a hydrogel network within the microcapsule. We further extend the utility of these microcapsules by demonstrating the enhanced retention of encapsulated fragrance in powder state.

The delivery of suspended active ingredients to a surface is a central function of numerous commercial cosmetic, drug, and agricultural formulations. Many products use liquid droplets as a delivery vehicle but, because interfacial tension keeps droplets spherical, these materials cannot exploit the benefits of anisotropic shape and shape change offered by solid colloids. In this work, individual droplet manipulation is used to produce viscoelastic droplets that can stably retain non-spherical shapes by balancing the Laplace pressure of the liquid-liquid interface with the elasticity of an internal crystalline network. A stability criterion is developed for idealized spherocylindrical droplets and shown to agree with experimental data for varying droplet size and rheology. Shape change can be induced in the anisotropic droplets by upsetting the balance of droplet interfacial tension and internal rheology. Using dilution to increase the interfacial tension shows that external stimuli can trigger collapse and shape change in these droplets. The droplets wrap around substrates during collapse, improving contact and adhesion. The model is used to develop design criteria for production of droplets with tunable response.