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Vapor deposition on polycrystalline films can lead to staggering levels ofcompressive stress, exceeding even the yield strength of the films.Mysteriously, a significant part of this stress has a reversible nature: itdisappears when the deposition is stopped and re-emerges upon resumption.Although numerous mechanisms have been proposed to explain these effects, theorigin of the phenomenon remains still unclear. The incorporation of atoms inthe grain boundaries is, to our opinion, the most likely mechanism, but therequired driving force for it has not yet been addressed. Therefore, instead ofsearching for a specific (atomic) incorporation process, we analyze, here, theentire film system using thermodynamic arguments only. We find that thetremendous stress levels observed in the experiments can be surprisinglyexplained by the flux induced entropic effects in the extremely dilute adatomgas on the surface alone. This thermodynamic evaluation delivers not only thenecessary basis for the adatom incorporation models, it even shows that themeasured stress values can be reached with low deposition fluxes. Finally,fully counterintuitive, we also show that the stress levels decrease, if thebarrier(s) for adatoms to reach the grain boundaries are decreased!

Thermodynamics of Deposition Flux dependent Intrinsic Film Stress