Highly regular laser-induced periodic surface structures (HR-LIPSS) have been fabricated on surfaces of Mo, steel alloy and Ti at a record processing speed on large areas and with a record regularity in the obtained sub-wavelength structures. The physical mechanisms governing LIPSS regularity are identified and linked with the decay length (i.e. the mean free path) of the excited surface electromagnetic waves (SEWs). The dispersion of the LIPSS orientation angle well correlates with the SEWs decay length: the shorter this length, the more regular are the LIPSS. A material dependent criterion for obtaining HR-LIPSS is proposed for a large variety of metallic materials. It has been found that decreasing the spot size close to the SEW decay length is a key for covering several cm² of material surface by HR-LIPSS in a few seconds. Theoretical predictions suggest that reducing the laser wavelength can provide the possibility of HR-LIPSS production on principally any metal. This new achievement in the unprecedented level of control over the laser-induced periodic structure formation makes this laser-writing technology to be flexible, robust and, hence, highly competitive for advanced industrial applications based on surface nanostructuring.

One of the remarkable capabilities of ultrashort polarized laser pulses is the generation of laser-induced periodic surface structures (LIPSS). The origin of this phenomenon is largely attributed to the interference of the incident laser wave and surface electromagnetic wave that creates a periodic absorption pattern. Although, commonly, LIPSS are produced by repetitive irradiation of the same area by multiple laser pulses in the regime of surface melting and resolidification, recent reports demonstrate the formation of LIPSS in the single-pulse irradiation regime at laser fluences well above the ablation threshold. In this paper, we report results of a large-scale molecular dynamics simulation aimed at providing insights into the mechanisms of single-pulse ablative LIPSS formation. The simulation performed for a Cr target reveals an interplay of material removal and redistribution in the course of spatially modulated ablation, leading to the transient formation of an elongated liquid wall extending up to $\sim 600$ nm above the surface of the target at the locations of the minima of the laser energy deposition. The upper part of the liquid wall disintegrates into droplets while the base of the wall solidifies on the time scale of $\sim 2$ ns, producing a $\sim 100$-nm-tall frozen surface feature extending above the level of the initial surface of the target. The properties of the surface region of the target are modified by the presence of high densities of dislocations and vacancies generated due to the rapid and highly nonequilibrium nature of the melting and resolidification processes. The insights into the LIPSS formation mechanisms may help in designing approaches for increasing the processing speed and improving the quality of the laser-patterned periodic surface structures.

Silicon is one of the most abundant materials which is used in many areas of modern research and technology. A variety of those applications require surface nanopatterning with minimum structure defects. However, the high-quality nanostructuring of large areas of silicon surface at industrially acceptable speed is still a challenge. Here, we report a rapid formation of highly regular laser-induced periodic surface structures (HR-LIPSS) in the regime of strong ablation by infrared femtosecond laser pulses at sub-MHz repetition rate. Parameters of the laser-surface interactions and obtained experimental results suggest an important role of electrostatically assisted bond softening in initiating the HR-LIPSS formation.