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Nature uses various activation mechanisms to program complex transformations in the shape and functionality of living organisms. Inspired by such natural events, we aimed to develop initially flat (i.e. two-dimensional) programmable materials that, when triggered by a stimulus such as temperature, could self-transform their shape into a complex three-dimensional geometry. A two-dimensional starting point enables full access to the surface, e.g. for (nano-)patterning purposes, which is not available in most other manufacturing techniques including additive manufacturing techniques and molding. We used different arrangements of bi- and multi-layers of a shape memory polymer (SMP) and hyperelastic polymers to program four basic modes of shape-shifting including self-rolling, self-twisting (self-helixing), combined self-rolling and self-wrinkling, and wave-like strips. The effects of various programming variables such as the thermomechanical properties of the hyperelastic layer, dimensions of the bi- and multi-layer strips, and activation temperature on the morphology of the resulting three-dimensional objects were studied experimentally and were found to cause as much as 10-fold change in the relevant dimensions. Some of the above-mentioned modes of shape-shifting were then integrated into other two-dimensional constructs to obtain self-twisting DNA-inspired structures, programmed pattern development in cellular solids, self-folding origami, and self-organizing fibers. Furthermore, the possibility of incorporating multiple surface patterns into one single piece of shape-transforming material is demonstrated using ultraviolet-cured photopolymers. Biomaterials & Tissue Biomechanic

Programming the shape-shifting of flat soft matter: from self-rolling/self-twisting materials to self-folding origami