Morphology and photoluminescence properties of silicon nanoparticles deposited in helium-nitrogen mixtures maintained at low residual pressures

We elaborated a technique of pulsed laser ablation in gas mixtures (He-N₂), maintained under residual pressures of 0.5–5 Torr to deposit silicon (Si)-based nanostructured films on a substrate. We show that the deposited films can exhibit strong photoluminescence (PL) emission with the position of peaks depending on the pressure of ambient gas and the ratio of gases in the mixture. Nanostructured films prepared in pure He gas exhibited a strong band in the infrared range (around 760 nm) and a weak band in the green range (550 nm), which were attributed to quantum-confined excitonic states in small Si nanocrystals and radiative transitions via the localized electronic states in silicon suboxide coating, respectively. In contrast, nanostructured films prepared in He-N₂ mixtures exhibited more intense "green-yellow" PL band centered at 580 nm, which was attributed to a radiative recombination in amorphous oxynitride (a-SiN_xO_y) coating of Si nanocrystals. We also present a detailed analysis of morphology of nanostructures Si-based films prepared by laser ablation. Finally, we show that the nanocrystals can be removed from the substrate and milled by ultrasound to form aqueous solutions of colloidal Si nanopartiles. The fabricated Si-based nanocrystals present a promising object for theranostics, combining imaging functionality based on PL emission and a series of therapy functionalities (photo and radiofrequency hyperthermia, photodynamic therapy).