First-principles study of the charge transfer and evolution of Si doping 2N2Ta islands adsorption on TaN (001) surfaces

Abstract The separation and aggregation of Si atoms around TaN grains during deposition of Ta–Si–N nanocomposite films were studied, and the adsorption energies, charge transfer and atomic partial density of state of Si–2N2Ta islands on the TaN (001) surface and diffusion energy of the islands during their evolution were evaluated using the first-principles method based on density functional theory (DFT). In the lowest total energy stable configuration, N and Ta atoms tended to combine to form 2N2Ta islands, whereas Si atoms tended to stay at a position diagonal to the Ta atom outside of the island. Si atoms entered the position of the missing N atom of the TaN island and formed a substitute solid solution during Ta–Si–N growth. The Si atoms of the solid solution in the island could be easily extruded by Ta- or N-rich island during the deposition process. The process of Si atom extrusion by a N atom which was the configuration of N–by–2Ta1N1Si island evolved into Si–by–2N2Ta island in rich N-atom. The process of Si atom was extruded by the Ta atom which was the configuration of Ta–by–2N1Ta1Si island evolved into Si–of–2Ta2N island, that reduced the total energy of island. The diffusion energies of these evolutions were 0.974 and 1.712 eV, respectively. The Si atoms and TaN grain phase tended to separate during the deposition process. Si atoms could give way to Ta and N atoms during the Ta–Si–N nanocomposite film deposition process.