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Ultrafast laser photoinscription of optical materials has seen a strong development in the recent years for a range of applications in integrated photonics. Fueled by its capability to confine energy in micro-domains of arbitrary geometries, it forecasts extensive potential in optical design. The process can locally modify the material structure and the electronic properties, changing in turn the refractive index. It thus lays down a powerful concept for three-dimensional modifications of materials, with the potential to design integrated optical functions. Using fused silica as model glass, this report discusses the physical mechanisms of photoinscription, outlining the possibility of refractive index engineering. We will review basic mechanisms of light propagation, excitation of matter, and energy relaxation concurring to material structural and photophysical modification. A dynamic perspective will be given, indicating relevant times for relaxing different forms of energy (electronic, thermal, etc.). The possibility to structure beyond diffraction limit will be explored, as well as the subsequent optical response of hybrid micro–nanostructures. Different irradiation geometries for photoinscription will be presented, pinpointing their potential to generate optical and photonic systems in three dimensions. Spatiotemporal pulse engineering can optimize the material response toward the achievement of accurate positive and negative index changes. An optimality concept can thus be defined for index design and present optimization concepts will be discussed. A particular potential derives from the utilization of non-diffractive beams with engineered dispersion. Finally, we indicate a range of application domains, from telecom to optofluidics and astrophotonics, outlining the potential of volume micro- and nanoprocessing.

Laser processing implies the generation of a material function defined by the shape and the size of the induced structures, being a collective effect of topography, morphology, and structural arrangement. A fundamental dimensional limit in laser processing is set by optical diffraction. Many material functions are yet defined at the micron scale, and laser microprocessing has become a mainstream development trend. Consequently, laser microscale applications have evolved significantly and developed into an industrial grade technology. New opportunities will nevertheless emerge from accessing the nanoscale. Advances in ultrafast laser processing technologies can enable unprecedented resolutions and processed feature sizes, with the prospect to bypass optical and thermal limits. We will review here the mechanisms of laser processing on extreme scales and the optical and material concepts allowing us to confine the energy beyond the optical limits. We will discuss direct focusing approaches, where the use of nonlinear and near-field effects has demonstrated strong capabilities for light confinement. We will argue that the control of material hydrodynamic response is the key to achieve ultimate resolution in laser processing. A specific structuring process couples both optical and material effects, the process of self-organization. We will discuss the newest results in surface and volume self-organization, indicating the dynamic interplay between light and matter evolution. Micron-sized and nanosized features can be combined into novel architectures and arrangements. We equally underline a new dimensional domain in processing accessible now using laser radiation, the sub-100-nm feature size. Potential application fields will be indicated as the structuring sizes approach the effective mean free path of transport phenomena.

A highly efficient drilling process is found in non-transparent metallic materials enabled by the use of non-diffractive ultrafast Bessel beams. Applied for deep drilling through a 200 μm-thick steel plate, the Bessel beam demonstrates twofold higher drilling efficiency compared to a Gaussian beam of similar fluence and spot size. Notwithstanding that surface ablation occurs with the same efficiency for both beams, the drilling booster results from a self-replication and reconstruction of the beam along the axis, driven by internal reflections within the crater at quasi-grazing incidence, bypassing potential obstacles. The mechanism is the consequence of an oblique wavevectors geometry with low angular dispersion and generates a propagation length beyond the projection range allowed by the geometry of the channel. With only the main lobe being selected by the channel entrance, side-wall reflection determines the refolding of the lobe on the axis, enhancing and replicating the beam multiple times inside the channel. The process is critically assisted by the reduction of particle shielding enabled by the intrinsic self-healing of the Bessel beam. Thus the drilling process is sustained in a way which is uniquely different from that of the conventional Gaussian beam, the latter being damped within its Rayleigh range. These mechanisms are supported and quantified by Finite Difference Time Domain calculations of the beam propagation. The results show key advantages for the quest towards efficient laser drilling and fabrication processes.

Ultrafast Bessel beams demonstrate a significant capacity of structuring transparent materials with a high degree of accuracy and exceptional aspect ratio. The ability to localize energy on the nanometer scale (bypassing the 100-nm milestone) makes them ideal tools for advanced laser nanoscale processing on surfaces and in the bulk. This allows to generate and combine micron and nano-sized features into hybrid structures that show novel functionalities. Their high aspect ratio and the accurate location can equally drive an efficient material modification and processing strategy on large dimensions. We review, here, the main concepts of generating and using Bessel non-diffractive beams and their remarkable features, discuss general characteristics of their interaction with matter in ablation and material modification regimes, and advocate their use for obtaining hybrid micro and nanoscale structures in two and three dimensions (2D and 3D) performing complex functions. High-throughput applications are indicated. The example list ranges from surface nanostructuring and laser cutting to ultrafast laser welding and the fabrication of 3D photonic systems embedded in the volume.

Cavitation in pure liquids and in liquids containing nanoparticles enables applications in mechanics, bio-medicine, and energy. Its evolution carries a significant interest. We describe the multiscale dynamic evolution of ultrafast-laser-induced cavitation in pure and gold-nanoparticles-doped liquids in one-dimensional geometries induced by non-diffractive ultrashort Bessel-Gauss laser beams. Covering the complete electronic and thermomechanical cycle, from the early plasma phase to bubble cavitation and collapse on ms timescales, we reconstitute, using time-resolved imaging with amplitude and phase sensitivity, the hydrodynamic phenomena concurring to bubble evolution. We indicate geometry-specific instabilities accompanying the collapse. The insertion of gold nanoparticles of 200 nm size has subtle effects in the process energetics. Albeit a moderate field enhancement minimizing the contribution to breakdown, the nanoparticles play a role in the overall relaxation dynamics of bubbles. The evolving bubble border in nanoparticles-containing liquids create a snow-plough effect that sweeps the nanoparticles at the gas liquid interface. This indicates that during the macroscopic cavity development, the nanoparticles were removed from the interaction region and dragged by the hydrodynamic movement. We thus shed light on the evolution of cavitation bubbles not triggered but perturbed by the presence of nanoparticles.

Optical feedback is often evoked in laser-induced periodic nanostructures. Visualizing the coupling between surfaces and light requires highly-resolved imaging methods. We propose in - situ structured-illumination-microscopy to observe ultrafast-laser-induced nanostructures during fabrication on metallic glass surfaces. This resolves the pulse-to-pulse development of periodic structures on a single irradiation site and indicates the optical feedback on surface topographies. Firstly, the quasi-constancy of the ripples pattern and the reinforcement of the surface relief with the same spatial positioning indicates a phase-locking mechanism that stabilizes and amplifies the ordered corrugation. Secondly, on sites with uncorrelated initial corrugation, we observe ripple patterns spatially in-phase. These feedback aspects rely on the electromagnetic interplay between the laser pulse and the surface relief, stabilizing the pattern in period and position. They are critically dependent on the space-time coherence of the exciting pulse. This suggests a modulation of energy according to the topography of the surface with a pattern phase imposed by the driving pulse. A scattering and interference model for ripple formation on surfaces supports the experimental observations. This relies on self-phase-stabilized far-field interaction between surface scattered wavelets and the incoming pulse front.

Slit-shaped laser beams focused in bulk optical materials can realize embedded waveguides with circular cross sections consisting of positive index change type I traces. In these kinds of waveguide traces, a peculiar periodical refractive index modulation was observed in type I waveguides with two different femtosecond lasers. The direction of refractive index modulation can be controlled with the slit configuration, and its period can be controlled by mechanical perturbation of the stages and the scanning speed. We argue that platform perturbation and dynamical thermal transport processes during the scan are generating factors in the appearance of this modulation. The embedded microstructures in waveguides can provide spectrum modulation, which may have potential applications in optical sensing, filtering, and phase control.

Using coupled electromagnetic and hydrodynamic calculations, we elucidate theoretically the topographic transition from a random metallic surface to a periodic sub-wavelength grating by ultrashort laser ablation. The origin of this transition lies in the successive selection of hybrid surface waves scattered by random nanoholes. Contrary to the common belief that surface plasmon polaritons play the dominant role in the process and define the grating periodicity, we show that both quasi-cylindrical and surface plasmon waves are involved, whereas the diversity in the resulting spacings /2– ( is the laser wavelength) is the manifestation of a broad frequency overlap of these waves, controlled by their relative phase shifts with respect to the plasmonic counterparts. The topography evolution imposes the dominant contribution to the surface sub-wavelength pattern by selecting the appropriate wave character from plasmonic modes to evanescent cylindrical waves. With the radiation dose, the grating periodicity exhibits a pronounced blue shift due to reinforced dipole–dipole coupling between the nanoholes and surface curvatures in the laser-processed area. This allows the creation of regular patterns with tunable periodicity.

The generation of an elliptical Bessel–Gauss beam has become a topic of interest in ultrafast laser processing of transparent materials because of its nearly non-diffractive elliptical central core. These beams can show potential in generating anisotropic structures down to the nanoscale and in producing asymmetries in the induced fields of thermo-mechanical constraints relevant for material structuring. However, maintaining the central core ellipticity is a challenge that requires further analysis, notably in the propagation behavior of phase anisotropies during the conical interference. This paper presents the controlled generation and propagation of a highly elliptical Bessel–Gauss beam using asymmetric phase-modulation technique. The study involves engineering different asymmetric phase holograms and analyzing their performances in terms of the non-diffractive property and uniformity of the generated beams. We indicate the presence in specific cases of diffraction and its influence on the invariance of the beam shape. The simulation results are in excellent agreement with the experimental results, which verifies the accuracy and reliability of our approach.

Excited by intense infrared ultrafast light pulses, a wide bandgap material undergoes nonlinear ionization, generating a high density of free electrons in conduction states. As a result, the electronic band structure is critically modified and the bandgap shrinks. This induces rapid changes in optical properties, dramatically affecting the absorption spectrum during light coupling to the dielectric surface or during nonlinear propagation inside the bulk. This study analyzes the structural behavior and the modification of the optical properties of laser‐excited silica glass at the molecular cluster level through first‐principles simulations. Employing density functional theory and the GW approximations for band structure under nonequilibrium conditions, alongside the Bethe–Salpeter equation, the dynamics of the optical properties of fused silica are comprehensively explored. The behavior of excited fused silica in a wide photon energy range (from a few to 20 eV) is thus predicted. Laser‐induced electron excitation triggers a redistribution of charges between oxygen and silicon atoms, accompanied by a significant increase in electronic pressure, local atomic structure rearrangement, and material expansion. Molecular dynamics simulations offer a temporal perspective on the excited state dynamics, unveiling the intricate interplay between electronic and atomic effects on bandgap evolution. The analysis sheds light on excitonic resonances, intraband and interband transitions in fused silica under ultrafast laser irradiation, providing valuable insights into its excited state behavior and optical properties. Calculations of optical properties of fused silica irradiated by ultrafast laser pulse. The contribution of both electronic and atomic factors to bandgap narrowing is estimated using density functional theory and GW approaches. The dielectric function Im[ε(ω)] is evaluated within the framework of the Bethe–Salpeter equation approximation and Drude model.