Controlling the properties of quantum dots at the atomic scale, such as dangling bonds, is a general motivation as they allow studying various nanoscale processes including atomic switches, charge storage, or low binding energy state interactions. Adjusting the coupling of individual silicon dangling bonds to form a 2D device having a defined function remains a challenge. Here, we exploit the anisotropic interactions between silicon dangling bonds on n-type doped Si(100):H surface to tune their hybridization. This process arises from interactions between the subsurface silicon network and dangling bonds inducing a combination of Jahn–Teller distortions and local charge ordering. A three-pointed star-shaped device prototype is designed. By changing the charge state of this device, its electronic properties are shown to switch reversibly from an ON to an OFF state via local change of its central gap. Our results provide a playground for the study of quantum information at the nanoscale.