Influence of nanostructure size on the luminescence behavior of silicon nanoparticle thin films

Abstract

We demonstrate the effect of particle size and quantum confinement on the luminescence properties of nanoscale silicon thin films. Thin films of agglomerated silicon nanoparticles are synthesized using pulsed laser ablation supersonic expansion. Following deposition, standard semiconductor processing techniques are employed to reduce the nanoparticle size. Films are oxidized both in air and chemically to reduce the silicon core dimensions, resulting in a shift of the luminescence emission peak to shorter wavelengths. Removal of the oxide using hydrofluoric acid (HF) results in further blueshifting of the luminescence, as does subsequent reoxidation in air and using nitric acid. The luminescence properties of samples are also studied as a function of excitation intensity. For room temperature excitation with a pulsed 355 nm source, a saturation of the photoluminescence intensity at high excitation intensity is observed, along with a blueshift of the peak PL wavelength. This behavior is found to persist at reduced temperature. A saturation of PL intensity, but no blueshift, is observed for high excitation intensity using a cw 488 nm source at room temperature. At reduced temperatures, no saturation of emission intensity occurs for high intensity 488 nm cw excitation. Both the irreversible shifting of the peak PL wavelength with size reducing treatments and the PL behavior at high excitation intensities indicate that quantum confinement determines the luminescence wavelength.