Periodic self-organization of matter beyond the diffraction limit is a puzzling phenomenon, typical both for surface and bulk ultrashort laser processing. Here we compare the mechanisms of periodic nanostructure formation on the surface and in the bulk of fused silica. We show that volume nanogratings and surface nanoripples having subwavelength periodicity and oriented perpendicular to the laser polarization share the same electromagnetic origin. The nanostructure orientation is defined by the near-field local enhancement in the vicinity of the inhomogeneous scattering centers. The periodicity is attributed to the coherent superposition of the waves scattered at inhomogeneities. Numerical calculations also support the multipulse accumulation nature of nanogratings formation on the surface and inside fused silica. Laser surface processing by multiple laser pulses promotes the transition from the high spatial frequency perpendicularly oriented nanoripples to the low spatial frequency ripples, parallel or perpendicular to the laser polarization. The latter structures also share the electromagnetic origin, but are related to the incident field interference with the scattered far-field of rough non-metallic or transiently metallic surfaces. The characteristic ripple appearances are predicted by combined electromagnetic and thermo-mechanical approaches and supported by SEM images of the final surface morphology and by time-resolved pump-probe diffraction measurements.
The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of semiconductors and dielectrics by linearly polarized high-intensity Ti:sapphire fs-laser pulses (τ ~100 fs, λ ~800 nm) is studied experimentally and theoretically. In the experiments, two different types of LIPSS exhibiting very different spatial periods are observed (socalled LSFL low spatial frequency LIPSS, and HSFL - high spatial frequency LIPSS), both having a different dependence on the incident laser fluence and pulse number per spot. The experimental results are analyzed by means of a new theoretical approach, which combines the generally accepted LIPSS theory of J. E. Sipe and co-workers [Phys. Rev. B 27, 1141-1154 (1983)] with a Drude model, in order to account for transient changes of the optical properties of the irradiated materials. The joint Sipe-Drude model is capable of explaining numerous aspects of fs-LIPSS formation, i.e., the orientation of the LIPSS, their fluence dependence as well as their spatial periods. The latter aspect is specifically demonstrated for silicon crystals, which show experimental LSFL periods Λ somewhat smaller than λ. This behaviour is caused by the excitation of surface plasmon polaritons, SPP, (once the initially semiconducting material turns to a metallic state upon formation of a dense free-electron-plasma in the material) and the subsequent interference between its electrical fields with that of the incident laser beam, resulting in a spatially modulated energy deposition at the surface.
Upon multi-pulse irradiation, a feedback mechanism, caused by the redshift of the resonance in a grating-assisted SPP excitation, is further reducing the LSFL spatial periods. The SPP-based mechanism of LSFL successfully explains the remarkably large range of LSFL periods between ~0.6 λ and λ.