Self-Rolling of Monolayer Graphene for Ultrasensitive Molecular Sensing

The controllable manipulation of graphene to create three-dimensional (3D) structures is an intriguing approach for favorably tuning its properties and creating new types of 3D devices. However, due to extremely low bending stiffnesses, it is rather challenging to construct monolayer graphene into stable 3D structures. Here, we demonstrate the stable formation of monolayer graphene microtubes with accompanying pre-patterned strain layers. The diameter of graphene microtubes can be effectively tuned by changing the thickness of the strain layers. Benefiting from a high surface-to-volume ratio of the tubular geometry, the 3D geometry leads to a prominent Raman enhancement, which was further applied to molecular sensing. The R6G molecules on graphene microtubes can be detected even for a concentration as low as 10^-11 M. We believe that this method can be a generalized way to realize the 3D tubular structure of other 2D materials.