Unveiling the Role of Substrate Interaction Types in Modulating Graphene’s Surface Adhesion

In this study, combining atomic force microscopy with density functional theory calculations, we quantitatively reveal how graphene-substrate coupling regulates the surface adhesion of graphene. We observe that chemisorbed graphene on Ni exhibits an adhesion force approximately 12% higher than that of physisorbed graphene on Cu.

This enhancement originates from the reduced graphene-metal separation, which amplifies the tip-substrate van der Waals interactions, and from increased interfacial charge transfer upon tip contact that further reinforces electrostatic attraction. This adhesion modulation also leads to altered surface functionality, as reflected by the progressively slower desorption of pyrene from Cu-supported graphene to Ni-supported graphene.