The self-induced growth of GaN nanocolumns (NCs) on SixN1−x/Si (111) is investigated as a function of the ratio of molecular to atomic nitrogen species generated via plasma assisted molecular beam epitaxy. Relative concentrations of the molecular and atomic species are calculated using optical emission spectroscopy. The growth rate (GR), diameter, and density of NCs are found to vary with the molecular to atomic nitrogen species relative abundance ratio within the plasma cavity. With increasing ratio, the GR and diameter of NCs increase while the density of NCs seems to be decreasing. The morphologies and the coalescence of GaN NCs exhibit a trend for molecular/atomic ratios up to 11, beyond which they still change but at a lower rate. The detrimental effect of taperedness of the NCs decreases with increasing molecular/atomic ratios. This is possibly because of reduction in radial growth in NCs due to increase in diffusivity of nitrogen species with increasing ratios.
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