Feedback-Driven Plasmonic-Thermal Route to Femtosecond-Laser-Induced Periodic Surface Structures in Silicon Indicated by Pump-Probe Scattering and Diffraction

Abstract

The self-organized formation of nanoscale laser-induced periodic surface structures (LIPSS) is still not fully understood with respect to the dynamics and interplay of contributing complex mechanisms. The transition from randomness to order and the specific role of nano-feedback are of fundamental interest because of their general aspects. In our study, the very first steps of the surface reconfiguration are demonstrated by analyzing the topology of evolving nano-crater maps. The evolution of spatial frequencies and directional arrangement indicate a feedback-driven adaptation of k-vectors to the required excitation conditions of elementary dipoles in the linearly polarized laser field. The time-dependent structure formation was studied by pump-probe diffraction and scattering experiments. The ratio of the contributions of characteristic light patterns enables plasmonic and non-plasmonic mechanisms to be distinguished, which subsequently act at distinctly different time scales. Recently developed multistage models for the dynamics of material modification are confirmed. The influence of accumulation effects is clearly demonstrated by characteristic changes in scattering and diffraction with an increasing number of preceding pulses. It is assumed that the thermal and plasmonic contributions to accumulation are coupled and thus generate spatially variable modifications.