Glassy, polydomain azobenzene liquid crystal polymer networks (azo-LCNs) have been synthesized, characterized, and modeled to understand composition dependence on large amplitude, bidirectional bending, and twisting deformation upon irradiation with linearly polarized blue-green (440–514 nm) light. These materials exhibit interesting properties for adaptive structure applications in which the shape of the photoresponsive material can be rapidly reconfigured with light. The basis for the photomechanical output observed in these materials is absorption of actinic light by azobenzene, which upon photoisomerization dictates an internal stress within the local polymer network. The photoinduced evolution of the underlying liquid crystal microstructure is manifested as macroscopic deformation of the glassy polymer film. Accordingly, this work examines the polarization-controlled bidirectional bending of highly concentrated azo-LCN materials and correlates the macroscopic output (observed as bending) to measured blocked stresses upon irradiation with blue-green light of varying polarization. The resulting photomechanical output is highly dependent on the concentration of crosslinked azobenzene mesogens employed in the formulation. Experiments that quantify photomechanical bending and photogenerated stress are compared to a large deformation photomechanical shell model to quantify the effect of polarized light interactions with the material during static and dynamic polarized light induced deformation. The model comparisons illustrate differences in internal photostrain and deformation rates as a function of composition and external mechanical constraints.
Cyclic loading conditions are commonly encountered in the applications of shape memory polymers (SMPs), where the cyclic characteristics of the materials determine their performance during the service life, such as deformation resistance, shape recovery speed and shape recovery ratio. Recent studies indicate that in addition to the physical damage or some other irreversible softening effects, the viscoelastic nature could also be another possible reason for the degraded cyclic behavior of SMPs. In this paper, we explore in detail the influence of the viscoelastic properties on the cyclic tension and shape memory (SM) behavior of an epoxy based amorphous thermosetting polymer. Cyclic experiments were conducted first, which show that although the epoxy material does not have any visible damage or irreversible softening effect during deformation, it still exhibits obvious degradation in the cyclic tension and SM behaviors. A linear multi-branched model is utilized to assist in the prediction and understanding of the mechanical responses of amorphous SMPs. Parametric studies based on the applied model suggest that the shape memory performance can be improved by adjusting programming and recovery conditions, such as lowering the loading rate, increasing the programming temperature, and reducing the holding time.
The inelastic deformation behavior of polymerization of monomeric reactants-15 (PMR-15) neat resin, a high-temperature thermoset polymer, was investigated at 288°C. The experimental program was designed to explore the influence of strain rate changes in the 10−6–10−3 s−1 range on tensile loading, unloading, and strain recovery behavior, as well as on the relaxation response of the material. The material exhibits positive, nonlinear strain rate sensitivity in monotonic loading. Nonlinear, “curved” stress-strain behavior during unloading is observed at all strain rates. The strain recovery at zero stress is profoundly affected by prior strain rate. The prior strain rate is also found to have a strong influence on relaxation behavior. The rest stresses measured at the termination of relaxation tests form the relaxation boundary, which resembles a nonlinear stress-strain curve. The results suggest that the inelastic behavior of the PMR-15 solid polymer at 288°C can be represented using a unified constitutive model with an overstress dependence of the inelastic rate of deformation. The experimental data are modeled with the viscoplasticity theory based on overstress. A systematic procedure for determining model parameters is presented and the model is employed to predict the response of the material under various test histories.
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