Date of Award


Document Type

Open Access Dissertation

Degree Name

Doctor of Philosophy (PhD)

Degree Program

Polymer Science and Engineering

First Advisor

Alfred J. Crosby

Second Advisor

Thomas J. McCarthy

Third Advisor

Narayanan Menon

Subject Categories



This work focuses on understanding deformation mechanisms and responsiveness associated with the wrinkling, folding, and snapping of thin polymer films. We demonstrated the use of elastic instabilities in confined regimes, such as the crumpling and snapping of surface attached sheets. We gained fundatmental insight into a thin film's ability to localize strain. By taking advantage of geometric strain localization we were able to develop new strategies for responsive surfaces that will have a broad impact on adhesive, optical, and patterning applications. Using the rapid closure of the Venus flytrap's leafets as dictated by the onset of a snap instability as motivation, we created surfaces with patterned structures to transition through a snap instability at a prescribed stress state. This mechanism causes surface topography to change over large lateral length scales and very short timescales. Changes in the stress state can be related to triggers such as chemical swelling, light-induced architecture transitions, mechanical pressure, or voltage. The primary advantages of the snap transition are that the magnitude of change, the rate of change, and the sensitivity to change can be dictated by a balance of materials properties and geometry. The patterned structures that exhibit these dynamics are elastomeric shells that geometrically localize strain and can snap between concave and convex curvatures. We have demonstrated the control of the microlens shell geometry and that the transition time follows scaling relationships presented for the Venus flytrap. Furthermore, the microlens arrays have been demonstrated as surfaces that can alter wettability. Using a similar novel processing technique, microarrays of freestanding elastomeric plates were placed in equibiaxial compression to fabricate crumpled morphologies with strain localized regions that are dicult to attain through traditional patterning techniques. The microstructures that form can be initially described using classical plate buckling theory for circular plates under an applied compressive strain. Upon the application of increasing compressive strain, axisymmetric microstructures undergo a secondary bifurcation into highly curved, nonaxisymmetric structures. The inherent interplay between geometry and strain in these systems provides a mechanism for generating responsiveness in the structures. By swelling the elastomeric plates with a compatible solvent, we demonstrated the microstructures ability to reversibly switch between axisymmetric and nonaxisymmetric geometries. To further explore the localization of strain in materials, we have fabricated sharply folded films of glassy, homogenous polymers directly on rigid substrates. The films were uniaxially compressed and buckle after delaminating from the substrate. As the applied strain is increased, we observed strain localization at the center of the delaminated features. We found that normally brittle, polystyrene films can accommodate excessive compressive strains without fracture by undergoing these strain localizing fold events. This technique provided a unique way to examine the curvature and stability of folded features, but was not adequate for understanding the onset of folding. By taking thin films, either glassy or elastomeric, and simply lifting them from the surface of water, we observed and quantified the wrinkle-to-fold transition in an axisymmetric geometry. The films initially wrinkle as they are lifted with a wavelength that is determined by the film thickness and material properties. The wrinkle-to-fold transition is analogous to the transition observed in uniaxially compressed films, but the axisymmetric geometry caused the fold to act as a disclination that increased the radial stress in the film, thereby decreasing the wavelength of the remaining wrinkles. Further straining the films caused the remaining wrinkles to collapse into a discrete number of folds that is independent of film thickness and material properties.

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