Controlling luminescent silicon nanoparticle emission produced by nanosecond pulsed laser ablation: role of interface defect states and crystallinity phase

In this study, we provide a systematic study on the origin of green and blue emission from luminescent silicon nanoparticles (Si-NPs) synthesized in water using a nanosecond pulsed laser ablation methodology. Here we report a direct one-step process to make ultra-small Si-NPs (∼3 nm mean size) by utilizing spiral beam scanning. In each ablation cycle, this scanning scheme collects generated nanoparticles towards the center and ablates them in subsequent cycles. Therefore, the resultant Si-NPs can reach very small sizes in a short time with high uniformity in their size distribution. Further, we investigate the effect of laser fluence on the emission properties of the obtained nanoparticles. For this aim, two different values of 60 mJ cm−2 and 30 mJ cm−2 laser fluences are employed to achieve green and blue emitting Si-NPs, respectively. Our results show that the emission spectrum for both blue and green Si-NPs has two main peaks at 426 nm and 520 nm, but their relative intensity ratios are different for these two cases. The findings of this study suggest that the blue emission originates from oxide related surface defects at the Si/SiOx interface, while the green emission stems from grain boundaries existing at the NP surface. We found that these two types of disorders can be controlled by tuning the laser power.