Graphene and other two-dimensional materials have unique physical and chemical properties of broad relevance. It has been suggested that transformation of such atomically planar materials to three-dimensional (3D) geometries by bending, wrinkling or folding could significantly alter their properties and lead to novel structures and devices with compact form factors, but strategies to enable such shape-change remain limited. Here, we report a benign thermally responsive method to fold and unfold monolayer graphene into predesigned, ordered 3D structures. The methodology involves the surface functionalization of monolayer graphene using non-covalent bonded mussel-inspired polydopamine and thermo-responsive poly(N-isopropylacrylamide) brushes. The functionalized graphene is micropatterned and self-folds into ordered 3D structures with reversible deformation under a full control by temperature. The structures are characterized using spectroscopy and microscopy, and self-folding is rationalized using a multi-scale molecular dynamics model of such functionalized graphene. Our work demonstrates the potential to design and synthesize ordered 3D graphene structures with predictable dynamics. We highlight applicability by encapsulating live cells and creating non-linear resistor and creased transistor devices.

Ultra-thin thermo-responsive self-folding 3D graphene

254th National Meeting (2017)

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