Quantitative analysis of plasma-enhanced chemical vapor deposition mechanisms: Quantum chemical and plasma-fluid dynamics investigation on tetraethoxysilane/O2 plasma

This study aimed to investigate the influence of reactive oxygen species (i.e., neutral O atom and O2+ ion) on deposition rates and film thickness uniformity in tetraethoxysilane (TEOS) plasma, utilizing a combination of plasma-fluid dynamic and quantum chemical (QC) simulations. The plasma simulations employed an improved model based on a previous study [H. Li et al., Jpn. J. Appl. Phys. 58, SEED06 (2019)], specifically tailored for a TEOS/O2/Ar/He gas mixture. In the QC simulations, both flat and step silicon oxide (SiO2) surfaces were employed to investigate the adsorption behavior of SiO molecules, the predominant silicon-containing species in TEOS plasma. These simulations also enabled the examination of the rates of SiO molecule adsorption on SiO2 surfaces, facilitating a direct comparison with the sticking coefficients utilized in the plasma simulation. The results of QC simulations revealed that SiO molecules exhibited a higher energetic preference for adsorption on step surfaces than on flat surfaces, resulting in the formation of new SiOH surface sites. Meanwhile, the plasma simulations demonstrated a strong correlation between the deposition rate and film thickness uniformity and the generation of oxygen species, specifically O atoms and O2+ ions, as well as their respective fluxes. This relationship takes precedence over the influence of TEOS or its fragments colliding with the surface. Notably, higher plasma source frequencies were found to enhance the production of atomic O, which contributed significantly to achieving higher deposition rates.