▎ 摘　　要

van der Waals (vdW) interactions play a central role in the surface-related physics and chemistry. Tuning of the correlated charge fluctuation in a vdW complex is a plausible way of modulating the molecules interaction at the atomic surface. Here, we report the vdW interaction tunability of the graphene CO, complex by combining the first-principles calculations with the vdW density functionals and the time evaluation measurements of CO, molecules adsorption/desorption on graphene under an external electric field. The field-dependent charge transfer within the complex unveils the controllable tuning of CO, from acceptor to donor. Meanwhile, the configuration of the adsorbed molecule, the equilibrium distance from graphene and O C-O bonding angle, is modified accordingly. The range of electrical tunability is a unique feature for each type of molecule.