Mechanics of light-activated network polymers

Mechanically responsive, environmentally activated polymers can undergo large, complex deformation in response to external stimuli such as thermal, luminous, and chemical changes to the environment. Light as a stimulus provides unique application potential because it allows for remote, rapid, and isothermal activation of the material with precise spatial control via existing optical technologies. While certain systems have received considerable attention, the state of the art of most light-activated polymers is limited to basic characterization and demonstrations. To make such materials available to the engineering and scientific communities, physically based theoretical and computational tools are required to guide experimental and design efforts that capitalize on their complex photo-mechanical couplings. The central objective of this thesis is to develop a multi-physics constitutive modeling framework to simulate the continuum scale, photo mechanical behavior of light-activated polymers and implement it into a finite element analysis setting. This framework is independent of specific underlying photo-stimulation mechanisms and is discussed in the context of photo-activated shape memory polymers and network rearranging polymers. Next, the framework is applied to the light-activated network rearranging polymer system, which is relaxed of stress upon irradiation with UV light, and a suite of characterization and application oriented experiments are carried out to calibrate and validate the model's predictive capabilities. The calibrated model is used to investigate several applications such as photo-activated stress relaxation of notched specimens, bending actuation, creep, the buckling of equi-biaxially deformed and irradiated films, and photomechanically formed 1D channels and ridges. Modeling creep involves additional complexity through simultaneous deformation and irradiation, and so the model framework is extended to cover such scenarios. Experiments, finite element analyses, and analytic solutions are developed to explore the phase space available to the experimentalist and design engineer for these different problems.