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.
Femtosecond laser-induced volume nanograting formation is numerically investigated. The developed model solves nonlinear Maxwell's equations coupled with multiple rate free carrier density equations in the presence of randomly distributed inhomogeneities in fused silica. As a result of the performed calculations, conduction band electron density is shown to form nanoplanes elongated perpendicular to the laser polarization. Two types of nanoplanes are identified. The structures of the first type have a characteristic period of the laser wavelength in glass and are attributed to the interference of the incident and the inhomogeneity-scattered light waves. Field components induced by coherent multiple scattering in directions perpendicular to the laser polarization are shown to be responsible for the formation of the second type of structures with a subwavelength periodicity. In this case, the influence of the inhomogeneity concentration on the period of nanoplanes is shown. The calculation results not only help to identify the physical origin of the self-organized nanogratings, but also explain their period and orientation.
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