Spectroscopic diagnostics and modeling of Ar/H2/CH4 microwave discharges used for nanocrystalline diamond deposition

In this paper Ar/H-2/CH4 microwave discharges used for nanocrystalline diamond chemical vapor deposition in a bell-jar cavity reactor were characterized by both experimental and modeling investigations. Discharges containing 1% CH4 and H-2 percentages ranging between 2% and 7% were analyzed as a function of the input microwave power under a pressure of 200 mbar. Emission spectroscopy and broadband absorption spectroscopy were carried out in the UV-visible spectral range in order to estimate the gas temperature and the C-2 density within the plasma. Infrared tunable diode laser absorption spectroscopy was achieved in order to measure the mole fractions of carbon-containing species such as CH4, C2H2, and C2H6. A thermochemical model was developed and used in order to estimate the discharge composition, the gas temperature, and the average electron energy in the frame of a quasihomogeneous plasma assumption. Experiments and calculations yielded consistent results with respect to plasma temperature and composition. A relatively high gas temperature ranging between 3000 and 4000 K is found for the investigated discharge conditions. The C-2 density estimated from both experiments and modeling are quite high compared with what is generally reported in the literature for the same kind of plasma system. It ranges between 10(13) and 10(14) cm(-3) in the investigated power range. Infrared absorption measurements and model predictions indicate quite low densities of methane and acetylene, while the atomic carbon density calculated by the model ranges between 10(13) and 10(15) cm(-3). The methane and hydrogen introduced in the feed gas are subject to a strong dissociation, which results in a surprisingly high H-atom population with mole fraction ranging between 0.04 and 0.16. Result analysis shows that the power coupling efficiency would range between 70% and 90%, which may at least explain the relatively high values obtained, as compared with those reported in the literature for similar discharges, for gas temperature and C-2 population. The high H-atom densities obtained in this work would indicate that growing nanocrystalline diamond films would experience a very high etching. Simulation results also confirm that sp species would play a key role in the surface chemistry that governs the diamond growth. (C) 2004 American Institute of Physics.