Experimental and computational study of the effect of 1 atm background gas on nanoparticle generation in femtosecond laser ablation of metals

Abstract Laser ablation of metal targets is actively used for generation of chemically clean nanoparticles for a broad range of practical applications. The processes involved in the nanoparticle formation at all relevant spatial and temporal scales are still not fully understood, making the precise control of the size and shape of the nanoparticles challenging. In this paper, a combination of molecular dynamics simulations and experiments is applied to investigate femtosecond laser ablation of aluminum targets in vacuum and in 1 atm argon background gas. The results of the simulations reveal a strong effect of the background gas environment on the initial plume expansion and evolution of the nanoparticle size distribution. The suppression of the generation of small/medium-size Al clusters and formation of a dense layer at the front of the expanding ablation plume, observed during the first nanosecond of the plume expansion in a simulation performed in the gas environment, have important implications on the characteristics of the nanoparticles deposited on a substrate and characterized in the experiments. The nanoparticles deposited in the gas environment are found to be more round-shaped and less flattened as compared to those deposited in vacuum. The nanoparticle size distributions exhibit power-law dependences with similar values of exponents obtained from fitting experimental and simulated data. Taken together, the results of this study suggest that the gas environment may be effectively used to control size and shape of nanoparticles generated by laser ablation.