In this thesis, we present a study on how droplets prepared in microfluidics can be used for fabrication of functional materials. We utilize the high degree of fluidic control enabled by miniaturizing the channels to achieve monodisperse single and multiple emulsion with high encapsulation efficiency. By engineering the interfaces of such emulsions and/or applying appropriate reactions, novel functional materials have been fabricated for encapsulation and release applications and for carrying out reactions in confined environments. Glass capillary microfluidics is used in the majority of the thesis. Glass offers excellent solvent resistance to most organic solvents needed for fabricating the desired materials.

In Chapter 1, we describe a double-emulsion-templated approach to form polymer vesicles, also known as polymersomes. By dissolving amphiphilic block copolymers in a volatile solvent, which forms the shell layer of double emulsions, polymersomes are formed after evaporation of the volatile solvent. In Chapter 2, we apply the same approach to fabricate phospholipid vesicles.

In Chapter 3, we investigate the physics of membrane formation at interfaces laden with amphiphilic diblock copolymers. In Chapter 4, we fabricate polymersomes with multiple compaitalents by using controlled double emulsion drops with multiple inner droplets as templates. In Chapter 5, we describe a non-microfluidic approach for fabricating similar polymersomes with large number of compartments. In Chapter 6, we show that the double-emulsion templated approach for forming polymersomes can be applied to two-dimensional stamped devices, which can be easily scaled up for production of large amount of polymersomes.

Apart from polymersomes, controlled emulsions can also be used for generating other functional materials. In Chapter 7, we use double emulsion drops as microreactors for fabricating particles of hydroxyapatite. In Chapter 8, we generate solid capsules by emulsifying a molten phase as the shell phase of double emulsions and subsequently cooling the emulsions. In Chapter 9, we describe several strategies that have been applied to form non-spherical particles using microfluidic emulsions as templates.

In Chapter 10, we demonstrate that controlled double emulsions cannot be formed at low interfacial tension between the shell and the continuous phases. Instead, compound jets with highly corrugated interfaces are observed.