Critical Time to Nucleation: Graphite and Silicon Nanoparticle Generation by Laser Ablation

Femtosecond laser ablation hydrodynamics has been analyzed numerically. The nucleation process of two materials (silicon and graphite) in an expanding plume produced by a femtosecond laser ablation is analyzed within the framework of the Zeldovich-Raizer theory (RZ theory). RZ theory is the most appropriate theory applicable to an expanding plume created by a femtosecond laser ablation and has been used to estimate the critical times in the evolution of nanoparticle formation. However, there is no experimental result to directly substantiate the theoretical model on a fundamental level. This paper gives an experimental approach to prove theoretical predictions of critical times to nucleation in laser-ablated graphite and silicon plumes. The critical time to nucleation deduced using the RZ theory was found to be in close agreement with pulse frequency at which fibrous nanoparticle aggregates start to form for both materials. We experimentally showed that the nanoparticle aggregates were produced consistently when the pulse frequency corresponding to the femtosecond laser time interval was shorter than the critical time to begin nucleation. Therefore the nucleation time acts as a threshold time length to begin nucleation.