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Here, upon systematic studies of femtosecond-laser processing ofmonocrystalline Si in oxidation-preventing methanol, we showed that theelectromagnetic processes dominating at initial steps of the progressivemorphology evolution define the onset of the hydrodynamic processes andresulting morphology upon subsequent multi-pulse exposure. In particular, underpromoted exposure quasi-regular subwavelength laser-induced periodic surfacestructures (LIPSSs) were justified to evolve through the template-assisteddevelopment of the Rayleigh-Plateau hydrodynamic instability in the moltenridges forming quasi-regular surface patterns with a supra-wavelengthperiodicity and preferential alignment along polarization direction of theincident light. Subsequent exposure promotes fusion-assisted morphologyrearrangement resulting in a spiky surface with a random orientation, yetconstant inter-structure distance correlated with initial LIPSS periodicity.Along with the insight onto the physical picture driving the morphologyevolution and supra-wavelength nanostructure formation, our experiments alsodemonstrated that the resulting quasi-regular and random spiky morphology canbe tailored by the intensity/polarization distribution of the incident laserbeam allowing on-demand surface nanotexturing with diverse hierarchical surfacemorphologies exhibiting reduced reflectivity in the visible and shortwave IRspectral ranges. Finally, we highlighted the practical attractiveness of thesuggested approach for improving near-IR photoresponse and expanding operationspectral range of vertical p-n junction Si photo-detector operating under roomtemperature and zero-bias conditions via single-step annealing-free lasernanopatterning of its surface.

Liquid-assisted laser nanotexturing of silicon: onset of hydrodynamic processes regulated by laser-induced periodic surface structures