Ultrashort-pulse laser ablation of gold thin film targets: Theory and experiment.

Abstract: Laser ablation of a gold thin film irradiated by ultrashort pulses is studied using molecular-dynamics simulations, and compared with that of a bulk target. A film thickness comparable to the ballistic electron depth in gold (≈100nm) is considered, evidencing a significant change of the temperature spatial profile inside the target material, which eventually influences the material decomposition. Particular emphasis is given to the process of nanoparticle generation. The simulations indicate a more uniform heating of the sample in the case of the thin film, which is accompanied by a more homogeneous size distribution of the nanoparticles produced in the ablation process. An experimental characterization of the ultrashort-pulse ablation process is also carried out. The produced nanoparticles are collected on suitable substrates, and atomic force microscopy analysis of less than one layer deposits is performed. An ≈2× narrowing of the nanoparticles equivalent to spherical diameter size distribution is observed in the case of ablation of the gold thin film, in fairly good agreement with the theoretical predictions. Moreover, interesting changes of the nanoparticle shape are evidenced, which are correlated to the changes in the nanoparticle ablation plume dynamics, as studied by time-gated imaging of its self-emission. Our findings suggest ultrashort-pulse laser ablation of thin films as a viable route to achieve a more uniform nanoparticle size distribution. [Copyright &y& Elsevier]