Multiscale electronic and thermomechanical dynamics in ultrafast nanoscale laser structuring of bulk fused silica.

ABSTRACT

We describe the evolution of ultrafast-laser-excited bulk fused silica over the entire relaxation range in one-dimensional geometries fixed by non-diffractive beams. Irradiation drives local embedded modifications of the refractive index in the form of index increase in densified glass or in the form of nanoscale voids. A dual spectroscopic and imaging investigation procedure is proposed, coupling electronic excitation and thermodynamic relaxation. Specific sub-ps and ns plasma decay times are respectively correlated to these index-related electronic and thermomechanical transformations. For the void formation stages, based on time-resolved spectral imaging, we first observe a dense transient plasma phase that departs from the case of a rarefied gas, and we indicate achievable temperatures in the excited matter in the 4,000-5,500 K range, extending for tens of ns. High-resolution speckle-free microscopy is then used to image optical signatures associated to structural transformations until the evolution stops. Multiscale imaging indicates characteristic timescales for plasma decay, heat diffusion, and void cavitation, pointing out key mechanisms of material transformation on the nanoscale in a range of processing conditions. If glass densification is driven by sub-ps electronic decay, for nanoscale structuring we advocate the passage through a long-living dense ionized phase that decomposes on tens of ns, triggering cavitation.