Understanding the mechanisms and controlling the possibilities of surface nanostructuring is of crucial interest for both fundamental science and application perspectives. Here, we report a direct experimental observation of laser-induced periodic surface structures (LIPSS) formed near a predesigned gold step edge following single-pulse femtosecond laser irradiation. Simulation results based on a hybrid atomistic-continuum model fully support the experimental observations. We experimentally detect nanosized surface features with a periodicity of ∼300 nm and heights of a few tens of nanometers. We identify two key components of single-pulse LIPSS formation: excitation of surface plasmon polaritons and material reorganization. Our results lay a solid foundation toward simple and efficient usage of light for innovative material processing technologies.
