Material-Dependent Evolution of Mechanical Folding Instabilities in Two-Dimensional Atomic Membranes

Inducing and controlling three-dimensional deformations in monolayer two-dimensional materials is important for applications from stretchable electronics to origami nanoelectromechanical systems. For these applications, it is critical to understand how the properties of different materials influence the morphologies of two-dimensional atomic membranes under mechanical loading. Here, we systematically investigate the evolution of mechanical folding instabilities in uniaxially compressed monolayer graphene and MoS₂ on a soft polydimethylsiloxane substrate. We examine the morphology of the compressed membranes using atomic force microscopy for compression from 0 to 33%. We find the membranes display roughly evenly spaced folds and observe two distinct stress release mechanisms under increasing compression. At low compression, the membranes delaminate to generate new folds. At higher compression, the membranes slip over the surface to enlarge existing folds. We observe a material-dependent transition between these two behaviors at a critical fold spacing of 1000 ± 250 nm for graphene and 550 ± 20 nm for MoS₂. We establish a simple shear-lag model which attributes the transition to a competition between static friction and adhesion and gives the maximum interfacial static friction on polydimethylsiloxane of 3.8 ± 0.8 MPa for graphene and 7.7 ± 2.5 MPa for MoS₂. Furthermore, in graphene, we observe an additional transition from standing folds to fallen folds at 8.5 ± 2.3 nm fold height. These results provide a framework to control the nanoscale fold structure of monolayer atomic membranes, which is a critical step in deterministically designing stretchable or foldable nanosystems based on two-dimensional materials.