Wallpapering-inspired spreading and wrinkling of atomically-thin materials

We propose a novel wallpapering-inspired strategy to create wrinkles in a desired location and direction of single-layer graphene (Gr). The key to controlling the wrinkles is to regulate the permeation and release of solution through a regular array of holes between the substrate surface and Gr-based thin membrane (Gr/Cu in the first stage and Gr in the second stage). Microscopic analysis showed that neighboring holes were interconnected by straightened wrinkles with a width of 300–500 nm and height of 10–20 nm, while surface corrugations (e.g., ripples and wrinkles) were suppressed on the planar regions surrounded by wrinkles. Wrinkling mechanism was further verified by in-situ optical microscopy and comparative analysis of Gr/Cu ripples and Gr wrinkles. Our approach is simple yet universally applicable to diverse types of thin membranes, thereby offering a robust and versatile route to engineering properties of atomically thin materials.