Multiscale, Hierarchical Patterning of Graphene by Conformal Wrinkling

This paper describes how delamination-free, hierarchical patterning of graphene can be achieved on prestrained thermoplastic sheets by surface wrinkling. Conformal contact between graphene and the substrate during strain relief was maintained by the presence of a soft skin layer, resulting in the uniform patterning of three-dimensional wrinkles over large areas (>cm²). The graphene wrinkle wavelength was tuned from the microscale to the nanoscale by controlling the thickness of the skin layer with 1 nm accuracy to realize a degree of control not possible by crumpling, which relies on delamination. Hierarchical patterning of the skin layers with varying thicknesses enabled multiscale graphene wrinkles with predetermined orientations to be formed. Significantly, hierarchical graphene wrinkles exhibited tunable mechanical stiffness at the nanoscale without compromising the macroscale electrical conductivity.