Molecular beam mass spectrometry and modelling of CH 4–CO 2 plasmas in relation with polycrystalline and nanocrystalline diamond deposition

Abstract

CH 4–CO 2 microwave plasmas have been studied by optical emission spectroscopy, microwave interferometry, Langmuir probing and molecular beam mass spectrometry. The variations of plasma parameters and the concentration variations of both stable species and radicals in the plasma had been reported previously as a function of the power density; the influence of the total inlet flow rate is reported here. While the power density influences directly the plasma kinetics, the flow rate changes the residence time in the plasma and then the degree of conversion of the chemical system that is the extent to which the gas composition moves toward its steady-state composition. This is studied by modelling of plasma kinetics taking into account the coupled fluid dynamics of the gaseous species and the gas-phase chemistry including electron dissociation and surface recombination at the reactor wall. The experimental and modelling studies are used for correlating: – the relative concentration of important hydrocarbon radicals and etching radicals in the plasma and the gradients of all these species in front of the surface; – to the deposition domain, the structure (polycrystalline or nanocrystalline) and the quality of diamond films, which is the ratio of sp 3 to (sp 3 + sp 2)-hybridized carbon in the film. All results evidence the plasma kinetic effect on the diamond deposition domain and the diamond deposition quality and structure, due to different degrees of conversion of the chemical system. The deposition of diamond coating from CH 4–CO 2 is shown to be a versatile process that permits deposition of a great variety of diamond films. However it requires particular attention because of the variation of the deposition conditions and then diamond quality and structure of the deposits depending on the extent of conversion of the inlet species to various intermediate and finally stable species formed in the plasma chemical system.