Combining aberration corrected high resolution transmission electron microscopy and density functional theory calculations we propose an explanation of the antisurfactant effect of Si in GaN growth. We identify the atomic structure of a Si delta-doped layer (commonly called SiN(x) mask) as a SiGaN(3) monolayer that resembles a √3×√3 R30° surface reconstruction containing one Si atom, one Ga atom, and a Ga vacancy (V(Ga)) in its unit cell. Our density functional theory calculations show that GaN growth on top of this SiGaN(3) layer is inhibited by forming an energetically unfavorable electrical dipole moment that increases with layer thickness and that is caused by charge transfer between cation dangling bonds at the surface to V(Ga) bound at subsurface sites.