Nanoscale Probing of Interaction in Atomically Thin Layered Materials

[Image: see text] We combine conductive atomic force microscopy (CAFM) and molecular dynamics (MD) simulations to reveal the interaction of atomically thin layered materials (ATLMs) down to nanoscale lateral dimension. The setup also allows quantifying, for the first time, the effect of layer number and electric field on the dielectric constant of ATLMs with few-layer down to monolayer thickness. Our CAFM-assisted electrostatic technique shows that high-quality mono- and bilayer graphene is reliably produced at significant yields only by the shear type of bond breaking between layers, whereas the normal type of bond breaking exhibits a very stochastic process mainly due to the coexistence of local delamination and interlayer twist. Our dielectric constant measurements also reveal a very weak dependence on the layer number and the electric field (up to our experimental limit of 0.1 V/Å), which is in contrast with theoretical reports. Owing to unexpectedly large variations in the screening ability of pristine monolayer graphene under ambient conditions, we further demonstrate that the effective dielectric constant of monolayer graphene can be engineered to provide a broad spectrum of dielectric responses (3.5–17) through oxidation and thermal annealing, thus confirming its much higher chemical reactivity than bilayer and few layers.