Controllable generation of large-scale highly regular gratings on Si films

The application of femtosecond laser-induced periodic surface texturing has significant potential in medicine, optics, tribology, and biology, among other areas. However, when irradiated by a large intense laser spot, the periodic structures usually exhibit an uncontrollable regularity, forming bifurcated patterns, thus limiting their widespread application. Irregularity originates from numerous independent branching seeds. The usual solution to this problem is to utilize the quasi-direct laser writing technique, that is, by limiting the laser beam size (diameter of <10 wavelengths) and scanning the beam or samples using 2D translation stages. Herein, we demonstrate an optical localization-induced nonlinear competition mechanism to solve this problem, which occurs at a fluence nearly one order of magnitude below the ablation threshold. Owing to the low intrinsic absorption of silicon and ultralow applied fluence, this mechanism ensures the self-selection of a single seed to initiate an array of bifurcated-free gratings under stationary irradiation with a large laser spot (diameter >100 wavelengths). Surprisingly, some unconventional complex patterns, such as radial, annular, and spiral gratings, can also be easily produced by structured light fields with unprecedented regularity. Their diameters reach up to >500 μm. Moreover, we can artificially control the initial seeding structure to further improve the regularity of the gratings, defined by dispersion in the ripple orientation angle in their 2D Fourier transform. As a result, the regularity in our experiments produced by a large laser spot is even higher than that scanned by a tiny beam. Controllable and highly regular ripples are beneficial to the structural coloring effects because they arise from the light diffraction by subwavelength gratings.