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Author ORCID Identifier


Open Access Dissertation

Document Type


Degree Name

Doctor of Philosophy (PhD)

Degree Program

Polymer Science and Engineering

Year Degree Awarded


Month Degree Awarded


First Advisor

Ryan C. Hayward

Subject Categories

Materials Chemistry


Engineering materials with the capability to transform energy from photons into mechanical work is an outstanding technical challenge with implications across myriad disciplines. Despite decades of work in this area, comprehensive understanding of how to prescribe shape change and work output in photoactive systems remains limited. To this end, this dissertation explores strategies to assemble photothermal and photochemical moieties in soft material systems to fabricate photoaddressable devices capable of specific shape changes upon illumination. Chapters 2 and 3 describe a methodology for spatially patterning plasmonic nanoparticles in liquid crystal elastomer fibers and sheets to specify local photothermally-induced strain profiles. Using this platform, devices capable of deployment into specific 3D configurations in response to both waveguided light and flood illumination are demonstrated. Next, to circumvent the inherent limitation of approaches based on photothermal effects, two new strategies for shape programming azobenzene-containing materials are explored for athermal photoactuation. In Chapter 4, a new material platform is presented that uses azobenzene incorporated into the backbone of polymers to modulate crystallinity on-demand via photoisomerization for next-generation shape memory systems. Next, host-guest cyclodextrin-azobenzene systems are shown in Chapter 5 to enable robust, re-programmable shape changes in hydrogels. Lastly, in Chapter 6 an outlook for the future of the field and an identification of areas in need of further study are presented.