Thermodynamics of deposition flux-dependent intrinsic film stress

Vapour deposition on polycrystalline films can lead to extremely high levels of compressive stress, exceeding even the yield strength of the films. A significant part of this stress has a reversible nature: it disappears when the deposition is stopped and re-emerges on resumption. Although the debate on the underlying mechanism still continues, insertion of atoms into grain boundaries seems to be the most likely one. However, the required driving force has not been identified. To address the problem we analyse, here, the entire film system using thermodynamic arguments. We find that the observed, tremendous stress levels can be explained by the flux-induced entropic effects in the extremely dilute adatom gas on the surface. Our analysis justifies any adatom incorporation model, as it delivers the underlying thermodynamic driving force. Counterintuitively, we also show that the stress levels decrease, if the barrier(s) for adatoms to reach the grain boundaries are decreased.