Nanosecond pulsed laser nanostructuring of Au thin films: Comparison between irradiation at low and atmospheric pressure

Highlights: • Background pressure plays an important role in NPs formation and its characteristics. • The NPs diameter and their size dispersion are smaller when irradiating in vacuum. • The plasmon resonance shifts ∼15 nm to higher frequencies when irradiating in vacuum. • Film partial ablation cannot be neglected for thickness in the range 40–80 nm. • In situ optical techniques monitor the timescale of the process and ablation dynamics. - Abstract: Au thin films with tens of nm in thickness deposited on glass substrates were irradiated with nanosecond UV (355 nm) laser pulses at atmospheric pressure and in vacuum conditions (∼600 and 10⁻⁵ Torr). We studied the effect of the laser fluence (200–400 mJ/cm²), thickness of the starting film (∼40–80 nm) and surrounding pressure on the partial ablation/evaporation of the films and the morphology of the produced nanoparticles (NPs). The dynamics of NPs formation was studied by measuring in real time the transmission of the samples upon continuous-wave laser exposure, and by means of probe beam deflection technique. The ejection of material from the film as a result of the irradiation was confirmed by time-resolved shadowgraphy technique. Experiments show that the NPs diameter and their size distribution are smaller when the irradiation is performed in vacuum regardless the laser fluence and thickness of the started film. It is also shown that the plasmon band shifts to higher frequencies with lower background pressure. The optical measurements show that the films melt and ablate during the laser pulse, but the transmission of the irradiated areas continues changing during tens of microseconds due to ejection of material and solidification of the remaining gold. Our results indicate that partial ablation cannot be neglected in nanostructuration by ns-pulsed irradiation of thin films when their thickness is in the studied range.