Annealing temperature and barrier thickness effect on the structural and optical properties of silicon nanocrystals/SiO2 superlattices

Abstract

The effect of the annealing temperature and the SiO2 barrier thickness of silicon nanocrystal (NC)/SiO2 superlattices (SLs) on their structural and optical properties is investigated. Energy-filtered transmission electron microscopy (TEM) revealed that the SL structure is maintained for annealing temperatures up to 1150 °C, with no variation on the nanostructure morphology for different SiO2 barrier thicknesses. Nevertheless, annealing temperatures as high as 1250 °C promote diffusion of Si atoms into the SiO2 barrier layers, which produces larger Si NCs and the loss of the NC size control expected from the SL approach. Complementary Raman scattering measurements corroborated these results for all the SiO2 and Si-rich oxynitride layer thicknesses. In addition, we observed an increasing crystalline fraction up to 1250 °C, which is related to a decreasing contribution of the suboxide transition layer between Si NCs and the SiO2 matrix due to the formation of larger NCs. Finally, photoluminescence measurements revealed that the emission of the superlattices exhibits a Gaussian-like lineshape with a maximum intensity after annealing at 1150 °C, indicating a high crystalline degree in good agreement with Raman results. Samples submitted to higher annealing temperatures display a progressive emission broadening, together with an increase in the central emission wavelength. Both effects are related to a progressive broadening of the size distribution with a larger mean size, in agreement with TEM observations. On the other hand, whereas the morphology of the Si NCs is unaffected by the SiO2 barrier thickness, the emission properties are slightly modified. These observed modifications in the emission lineshape allow monitoring the precipitation process of Si NCs in a direct non-destructive way. All these experimental results evidence that an annealing temperature of 1150 °C and 1-nm SiO2 barrier can be reached whilst preserving the SL structure, being thus the optimal structural SL parameters for their use in optoelectronics.