Femtosecond pulse train-facilitated periodic nanostructuring on TiN films via laser-oxidation

Laser-induced periodic surface structure is a universal phenomenon observed when solid materials are irradiated with pulsed lasers. Typically, these structures are generated using Gaussian pulses. Here, we investigate the formation of periodic nanostructures on titanium nitride thin films using two different laser sources: Gaussian pulses and femtosecond pulse trains generated through a Fabry-Perot cavity. Our findings indicate that the formation of self-organized nanostructures on the thin films can occur through either laser-induced oxidation or laser ablation processes, depending on laser fluence, scanning speed, and pulse duration. Interestingly, when utilizing femtosecond pulse trains, we observe that the range of laser fluence thresholds for oxidative nanostructure formation is significantly wider compared to Gaussian pulses. To comprehend the underlying mechanisms driving these observations, we employ a two-temperature model to calculate the ultrafast dynamics of hot electrons when exposed to laser irradiation. Our results reveal that the initial sub-pulse generates a substantial population of hot electrons, exciting surface plasmons and resulting in the creation of a periodic energy distribution. Before these hot electrons can dissipate, subsequent sub-pulses reach the thin film, re-exciting a large number of hot electrons. Consequently, the periodic energy distribution persists for an extended duration, creating more favorable conditions for the formation of periodic oxidative nanostructures when using pulse trains. These findings contribute to a comprehensive understanding of the mechanisms involved in the formation of periodic nanostructures under femtosecond laser irradiation.