Photoluminescence of As-Grown Silicon Nanocrystals Embedded in Silicon Nitride: Influence of Atomic Hydrogen Abundance

Silicon nanocrystals embedded in silicon nitride films were grown by direct plasma enhanced chemical vapor deposition at 300 °C, using mixtures of SiH₂Cl₂/NH₃/H₂/Ar. The films composition and chemical stability was tested by Fourier Transform Infrared Spectroscopy and Rutherford Backscattering Spectroscopy. The influence of hydrogen abundance during the deposition process on the photoluminescence of as-grown samples was studied as a function of the radiofrequency power and hydrogen dilution flow rate. In situ Optical Emission Spectroscopy allowed the diagnostic of the species in the plasma region and their general trends as a function of the radiofrequency power. The changes in the hydrogen content and silicon incorporation to the film as a function of the radiofrequency power were discussed in terms of silicon nanocrystals formation and growth in the silicon nitride matrix. The photoluminescence emission from the as-grown samples was found to red-shift with increasing hydrogen abundance. This observation is consistent with the increase in silicon content associated to nc-Si of larger size. On the other hand, the photoluminescence intensity was observed to decrease for very high radiofrequency powers and hydrogen dilutions. High Resolution Transmission Electron Microscopy confirmed the presence of silicon nanocrystals embedded in the amorphous silicon nitride matrix and allowed the correlation between the nanocrystals size and the photoluminescence emission energy using the quantum confinement model.