Boron nitride-graphene nanocapacitor and the origins of anomalous size-dependent increase of capacitance

Conventional wisdom suggests that decreasing dimensions of dielectric materials (e.g., thickness of a film) should yield increasing capacitance. However, the quantum capacitance and the so-called "dead-layer" effect often conspire to decrease the capacitance of extremely small nanostructures, which is in sharp contrast to what is expected from classical electrostatics. Very recently, first-principles studies have predicted that a nanocapacitor made of graphene and hexagonal boron nitride (h-BN) films can achieve superior capacitor properties. In this work, we fabricate the thinnest possible nanocapacitor system, essentially consisting of only monolayer materials: h-BN with graphene electrodes. We experimentally demonstrate an increase of the h-BN films' permittivity in different stack structures combined with graphene. We find a significant increase in capacitance below a thickness of ∼5 nm, more than 100% of what is predicted by classical electrostatics. Detailed quantum mechanical calculations suggest that this anomalous increase in capacitance is due to the negative quantum capacitance that this particular materials system exhibits.