Dépôt de films d'oxyde de silicium par vaporisation sous vide : dynamique moléculaire et expériences

Abstract : Silica thin films are widely used as low index layers in antireflective coatings. In the ophthalmic industry, they are deposited at ambient temperature, by electron beam vaporization. This process generates large compressive stresses which make the coatings susceptible to damage. It is thus crucial to understand how these stresses emerge. However, this problem is highly complex because many process parameters may play a role: substrate and residual gas properties, characteristics of the deposition chamber, of the electron gun, growth rate,… Moreover, these parameters may depend on each other and affect several phenomena at the same time. In this thesis, numerical simulations and experiments are performed in order to identifiy the mechanisms responsible for the generation of compressive stresses during film growth. The experiments reveal three regimes of growth, depending on the residual gas pressure. Near ultra high vacuum, where the effect of residual gas is negligible, films grow under compression. Then, as pressure increases, incorporation of gas species in the films slightly compresses them. Eventually, when pressure is high enough so that vaporized particles are slowed down by collisions with gas particles, the level of compression significantly decreases; this rapidly masks the incorporation effect. Molecular dynamics simulations allow us to explore the ideal vacuum limit. By depositing silica films in a vast ensemble of conditions, we find that their compressive state of stress is solely controlled by the mean kinetic energy of incident particles. Comparison with experiments suggests that this energy is equal to a few eV, which is at least ten times greater than predictions from the literature on deposition. This unexpected result leads us to refute the idea that electron beam vaporization would be equivalent to simple themal heating. We confirm this experimentally, by comparing films deposited from silicon monoxide either thermally evaporated or vaporized using an electron beam: the formers grow under tension while the latters under compression. Finally, we explain the ejection of particles of a few eV as coming from the very low electrical conductivity of silica: under electronic irradiation, charges accumulate at its surface and accelerate the charged vaporized particles by Coulombian repulsions
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Simon Gelin. Dépôt de films d'oxyde de silicium par vaporisation sous vide : dynamique moléculaire et expériences. Matériaux. Université Paris-Est, 2016. Français. ⟨NNT : 2016PESC1117⟩. ⟨tel-01459287⟩

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