International audienceUltrashort laser pulses can modify the inner structure of fused silica, generating refractive index changes varying from soft positive (type I) light guiding forms to negative (type II) values with void presence and anisotropic sub-wavelength modulation. We investigate electronic and structural material changes in the type I to type II transition via coherent and incoherent secondary light emission reflecting free carrier behavior and post-irradiation material relaxation in the index change patterns. Using phase contrast microscopy, photoluminescence, and Raman spectroscopy, we determine in a space-resolved manner defect formation, redistribution and spatial segregation, and glass network reorganization paths in conditions marking the changeover between type I and type II photoinscription regimes. We first show characteristic patterns of second harmonic generation in type I and type II traces, indicating the collective involvement of free carriers and polarization memory. Second, incoherent photoemission from resonantly and non-resonantly excited defect states reveals accumulation of non-bridging oxygen hole centers (NBOHCs) in positive index domains and oxygen deficiency centers (ODCs) with O 2 ions segregation in voidlike regions and in the nanostructured domains, reflecting the interaction strength. Complementary Raman investigations put into evidence signatures of the different environments where photochemical densification (bond rearrangements) and mechanical effects can be indicated. NBOHCs setting in before visible index changes serve as precursors for subsequent compaction build-up, indicating a scenario of cold, defect-assisted densification for the soft type I irradiation regime. Additionally, we observe hydrodynamic effects and severe bond-breaking in type II zones with indications of phase transition. These observations illuminate densification paths in fused silica in low power irradiation regimes, and equally in energetic ranges, characterized by the onset of thermo-mechanical effects

International audienceWe report single-shot, high aspect ratio nanovoid fabrication in bulk fused silica using zeroth order chirp-controlled ultrafast laser Bessel beams. We identify a unique laser pulse length and energy dependence of the physical characteristics of machined structures over which nanovoids of diameter in the range 200-400 nm and aspect ratios exceeding 1000 can be fabricated. A mechanism based on the axial energy deposition of nonlinear ultrashort Bessel beams and subsequent material densification or rarefaction in fused silica is proposed, intricating the non-diffractive nature with the diffusing character of laser-generated free carriers. Fluid flow through nanochannel is also demonstrate

International audienceThumbnail image of graphical abstractNondiffractive ultrafast optical beams with quasi-stationary characteristics enable new regimes and scales in light-matter interactions. We discuss the action of ultrashort Bessel laser beams in bulk fused silica, emphasizing excitation dynamics with energy localization beyond diffraction limit. We shed light on relaxation channels leading to one-dimensional structures with nanoscale sections and morphologies ranging from densified matter to nanosized cavities. Space- and time-resolved absorption and phase-contrast microscopy reveals two main carrier relaxation paths. Fast exciton trapping in self-induced matrix deformations results in positive index contrast driven by swift accumulation of non-bridging oxygen hole centers and defect-driven structural rearrangements. High excitation densities determine thermomechanical paths, with onset of phase transitions and the release of pressure waves. High-aspect-ratio nanosized channels are thus created via rarefaction and liquid cavitation, accompanied by molecular decomposition and generation of oxygen deficiency. The characteristic electronic relaxation identifies the nature of structural transitions up to the onset of phase transformation. Temporal pulse dispersion regulation allows driving unique carrier dynamics with precise control over energy deposition down to the 100 nm scale. Extreme high-aspect-ratio uniform void structures can thus be fabricated in conditions of sub-micron transverse light confinemen

International audienceThe spatio-temporal design of ultrafast laser excitation can have a determinant influence on the physical and engineering aspects of laser-matter interactions,with the potential of upgrading laser processing effects. Energy relaxation channels can be synergetically stimulated as the energy delivery rate is synchronized with the material response on ps timescales. Experimental and theoretical loops based on the temporal design of laser irradiation and rapid monitoring of irradiation effects are, therefore, able to predict and determine ideal optimal laser pulse forms for specific ablation objectives.We illustrate this with examples on manipulating the thermodynamic relaxation pathways impacting the ablation products and nanostructuring of bulk and surfaces using longer pulse envelopes. Some of the potential control factors will be pointed out. At the same time the spatial character can dramatically influence the development of laser interaction. We discuss spatial beam engineering examples such as parallel and non-diffractive approaches designed for highthroughput, high-accuracy processing events

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The laser-induced damage threshold (LIDT) of optical components is one of the major constraints in developing high-power ultrafast laser systems. Multi-layer dielectric (MLD) coatings-based optical components are key parts of high-power laser systems because of their high damage resistance. Therefore, understanding and characterizing the laser-induced damage of MLD coatings are of paramount importance for developing ultrahigh-intensity laser systems. In this article, we overview the possible femtosecond laser damage mechanisms through damage morphologies in various MLD optical coatings tested in our facility. To evaluate the major contributions to the coating failure, different LIDT test methods (R-on-1, ISO S-on-1 and Raster Scan) were carried out for a high reflective hybrid Ta2O5/HfO2/SiO2 MLD mirror coating at a pulse duration of 37 fs. Different LIDT test methods were compared due to the fact that each test method exposes the different underlying damage mechanisms. For instance, the ISO S-on-1 test at a higher number of laser pulses can bring out the fatigue effects, whereas the Raster Scan method can reveal the non-uniform defect clusters in the optical coating. The measured LIDT values on the sample surface for the tested coating in three test methods are 1.1 J/cm2 (R-on-1), 0.9 J/cm2 (100k-on-1) and 0.6 J/cm2 (Raster Scan) at an angle of incidence of 45 deg. The presented results reveal that the performance of the tested sample is limited by coating defects rather than fatigue effects. Hence, the Raster Scan method is found to be most accurate for the tested coating in evaluating the damage threshold for practical applications. Importantly, this study demonstrates that the testing of different LIDT test protocols is necessary in femtosecond regime to assess the key mechanisms to the coating failure.

The latest advances in petawatt laser technology within the ELI Beamlines project have stimulated the development of large surface area dielectrically coated mirrors meeting all demanding requirements for guiding the compressed 30 J, 25 fs HAPLS laser beam at 10 Hz repetition rate and a center wavelength of 810 nm entirely in vacuum. We describe the production and evaluation of Ta2O5/HfO2/SiO2 ion beam sputtered coated (440 × 290 × 75) mm3 beam transport mirrors. No crazing was observed after thirty vacuum-air cycles. A laser induced damage threshold of 0.76 J/cm2 (fluence on mirror surface) was achieved and maintained at high shot rates.