An innovative kinetic model allowing insight in the moderate temperature chemical vapor deposition of silicon oxynitride films from tris(dimethylsilyl)amine

Konstantina Christina Topka (1, 2) , Hugues Vergnes (2) , Tryfon Tsiros (2) , Paris Papavasileiou (1) , Laura Decosterd (1) , Babacar Diallo (3) , François Senocq (1) , Diane Samelor (1) , Nadia Pellerin (3) , Marie-Joëlle Menu (1) , Constantin Vahlas (1) , Brigitte Caussat (2)

1 CIRIMAT - Centre interuniversitaire de recherche et d'ingenierie des matériaux
2 LGC - Laboratoire de Génie Chimique
3 CEMHTI - Conditions Extrêmes et Matériaux : Haute Température et Irradiation

An apparent kinetic model is developed for a novel chemical vapor deposition (CVD) process of silicon oxynitride (SiO x N y) films from tris(dimethylsilyl)amine (TDMSA) and O 2 , operating at moderate temperature (600-650 • C) and at atmospheric pressure. The definition of reaction pathways and the extraction of kinetic information is based on recently reported results of the gas phase composition, complemented by solid phase characteristics obtained by spectroscopic ellipsometry (SE) and ion beam analyses (IBA). Incorporation of carbon (up to 20 at. %) is considered alongside nitrogen (up to 25 at.%) for variable O 2 flow rates (0.3-1.2 sccm). This combined gasand solid-phase analysis is utilized to identify the main gaseous species and provide insight into the deposition mechanism. A silicon-and a nitrogen-centered radical intermediates are considered as the primary species of the mechanism, based on evidence from gas phase characterizations. A third, fictitious, nitrogen-and carboncontaining molecule is also conceptualized to account for carbon incorporation. Eight chemical reactions are defined alongside their respective kinetic parameters and are implemented in the ANSYS® FLUENT® computational fluid dynamics (CFD) code. Upon validation, the model allows for the successful prediction of local deposition rates and SiO x N y film composition containing non-negligible carbon, marking it as the first kinetic model able to represent the main chemical mechanisms involved in the CVD of a four-component material. The reported combined approach could be applied to other existing or new CVD chemistries forming multicomponent thin films, favoring their implementation in original applications.

Mots clés: Computational fluid dynamics; Kinetic model; Silanamine precursor; Chemical vapor deposition; Silicon oxynitride; Experimental validation

Domaines: Matériaux; Matériaux

Konstantina Christina Topka, Hugues Vergnes, Tryfon Tsiros, Paris Papavasileiou, Laura Decosterd, et al.. An innovative kinetic model allowing insight in the moderate temperature chemical vapor deposition of silicon oxynitride films from tris(dimethylsilyl)amine. Chemical Engineering Journal, 2021, 431, pp.133350. ⟨10.1016/j.cej.2021.133350⟩. ⟨hal-03514135⟩