Time-dependent Monte Carlo simulations of surface reactions in diamond film growth

Diamond is an interesting material for applications that require properties such as mechanic resistance, high thermal conductivity, low electric conductivity, optical transparency, and high electron hole mobility. Much development of the techniques leading to diamond film deposition has been achieved in the last decade. However, the prices for commercial diamond films are not competitive for many potential applications and understanding of the chemical details leading to film growth is needed.; This dissertation presents three-dimensional time-dependent Monte Carlo simulations of diamond film growth with methyl as diamond precursor on a (100) surface based on a detailed chemical kinetics mechanism that includes surface migration and etching reactions.; Migration reactions were observed to significantly affect the overall kinetic behavior of the deposition process. Results showed that with migration included the computed growth rates were in the vicinity of the experimental results whereas the numerical predictions were more than one order of magnitude lower than the experimental values when migration reactions were excluded from the mechanism.; Etching was shown to be important in producing continuous film growth. The main role of etching in the overall behavior of the mechanism was to prevent the surface from being in an unfavorable-to-growth condition.; Results from the calculations showed that the higher the atomic hydrogen or methyl concentrations, the larger the growth rates. The simulations with different substrate temperatures did not produce the peak in growth rate observed in experimental studies. The kinetics of the sp2 carbon needs to be included for a complete description of the temperature effect.; All domain sizes resulted in pyramid-like intermediate showing the appearance of {lcub}111{rcub} planes during the deposition process on a {lcub}100{rcub} plane. This is in agreement with experimental observations. However, the perfect dimer-row {lcub}100{rcub} planes observed in experiments were not observed during the growth simulations. Simulations only with etching reactions acting on the surface generated smooth dimer-row surfaces, offering an alternative explanation for the experimental dimer-row images. The growth, in fact, would not proceed through dimer row domains. The dimer row domains observed are produced through an etching-only environment for a short period of time after the film deposition.