Poly(ionic liquid)s (PILs) with an intrinsically conducting pyrrole polymer (ICP) backbone were synthesized and utilized as novel dispersants of carbon nanotubes (CNTs) in various polar and nonpolar solvents. This is due to their highly tunable nature, in which the anions can be easily exchanged to form PILs of varying polarity but with the same polycation. These CNT dispersions were exceedingly stable over many months, and with the addition of hexane, Pickering emulsions with the PIL-stabilized CNTs at the droplet interfaces were formed. Depending on the hydrophobicity of the PIL, hexane-in-water and hexane-in-acetonitrile emulsions were formed, the latter marking the first non-aqueous stabilized-CNT emulsions and corresponding CNT-in-acetonitrile dispersion, further advancing the processability of CNTs. The PIL-stabilized CNT Pickering emulsion droplets generated hollow conductive particles by subsequent drying of the emulsions. With the emulsion templating, the hollow shells can be used as a payload carrier, depending on the solubility of the payload in the droplet phase of the emulsion. This was demonstrated with silicon nanoparticles, which have limited solubility in aqueous environments, but great scientific interest due to their potential electrochemical applications. Overall, this work explored a new class of efficient PIL-ICP hybrid stabilizers with tunable hydrophobicity, offering extended stability of carbon nanotube dispersions with novel applications in hollow particle formation via Pickering emulsion templating and in placing payloads into the shells.

Environmentally responsive hydrogels are one interesting class of soft materials. Due to their remarkable responsiveness to stimuli such as temperature, pH, or light, they have attracted widespread attention in many fields. However, certain functionality of these materials alone is often limited in comparison to other materials such as silicon; thus, there is a need to integrate soft and hard materials for the advancement of environmental-ly responsive materials.

Conventional hydrogels lack good mechanical properties and have inherently slow response time, important characteristics which must be improved before the hydrogels can be integrated with silicon. In the present dissertation work, both these important attrib-utes of a temperature responsive hydrogel, poly(N-isopropylacrylamide) (PNIPAAm), were improved by adopting a low temperature polymerization process and adding a sili-cate compound, tetramethyl orthosilicate. Furthermore, the transition temperature was modulated by adjusting the media quality in which the hydrogels were equilibrated, e.g. by adding a co-solvent (methanol) or an anionic surfactant (sodium dodecyl sulfate). In-terestingly, the results revealed that, based on the hydrogels’ porosity, there were appre-ciable differences when the PNIPAAm hydrogels interacted with the media molecules.

Next, an adhesion mechanism was developed in order to transfer silicon thin film onto the hydrogel surface. This integration provided a means of mechanical buckling of the thin silicon film due to changes in environmental stimuli (e.g., temperature, pH). We also investigated how novel transfer printing techniques could be used to generate pat-terned deformation of silicon thin film when integrated on a planar hydrogel substrate. Furthermore, we explore multilayer hybrid hydrogel structures formed by the integration of different types of hydrogels that have tunable curvatures under the influence of differ-ent stimuli. Silicon thin film integration on such tunable curvature substrates reveal char-acteristic reversible buckling of the thin film in the presence of multiple stimuli.

Finally, different approaches of incorporating visible light response in PNIPAAm are discussed. Specifically, a chemical chromophore- spirobenzopyran was synthesized and integrated through chemical cross-linking into the PNIPAAm hydrogels. Further, methods of improving the light response and mechanical properties were also demonstrat-ed. Interestingly, such a system was shown to have potential application as light modulated topography altering system