Nucleation and growth of Si nanoparticles under different pulse repetition rates without the baffle for nanosecond pulsed laser-ablated deposition

In this article, Si nanoparticle (NP) films were prepared by pulsed laser ablation (PLA) in the argon atmosphere of 10 Pa at room temperature under different pulse repetition rates from 1 to 40 Hz without the baffle. Different from the conventional PLA method, the substrates were placed below and parallel to the ablated plume axis. The obtained films containing NPs were characterized by scanning electron microscopy and Raman spectrometer. The experimental results under constant laser fluence demonstrate the strong dependence of the mean size and the area number density of NPs on the repetition rate. Specifically, with the increase of pulse repetition rate, the mean size of the NPs in the film first decreases and reaches its minimum at 20 Hz, and then increases after 20 Hz, and decreases again till 40 Hz. The area number density shows the contrary trend versus mean size. The in situ diagnostic results of Langmuir probe denote the ablated Si ion density increases monotonously with the increase of repetition rate, while the temperature is almost constant. Combining with the nucleation probability, the growth/aggregation duration of NPs in the “nucleation region” and the effect of the baffle, the influence of pulse repetition rate on the formation of NPs is addressed. It is found that the repetition rate impacts the growth modes of NPs (i.e., growth and aggregation). 1–20, 20–30, and 30–40 Hz, respectively, correspond to growth-, aggregation-, and growth-controlled rate ranges without the baffle; however, 1–10, 10–20, and 20–40 Hz, respectively, correspond to growth-controlled, aggregation/growth-coexisted, and aggregation-controlled rate ranges with the baffle.