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The prospect of employing nanophotonic methods for controlling photon–electron interactions has ignited substantial interest within the particle accelerator community. Silicon-based integrated dielectric laser acceleration (DLA) has emerged as a viable option by leveraging localized photonic effects to emit, accelerate, and measure electron bunches using exclusively light. Here, using highly regular nanopatterning over large areas while preserving the crystalline structure of silicon is imperative to enhance the efficiency and yield of photon-electron effects. While several established fabrication techniques may be used to produce the required silicon nanostructures, alternative techniques are beneficial to enhance scalability, simplicity and cost-efficiency. In this study, we demonstrate the nano-synthesis of silicon structures over arbitrarily large areas utilizing exclusively deep ultraviolet (DUV) ultrafast laser excitation. This approach delivers highly concentrated electromagnetic energy to the material, thus producing nanostructures with features well beyond the diffraction limit. At the core of our demonstration is the production of silicon laser-induced surface structures with an exceptionally high aspect-ratio -reaching a height of more than 100 nm- for a nanostructure periodicity of 250 nm. This result is attained by exploiting a positive feedback effect on the locally enhanced laser electric field as the surface morphology dynamically emerges, in combination with the material properties at DUV wavelengths. We also observe strong nanopattern hybridization yielding intricate 2D structural features as the onset of amorphization takes place at high laser pulse fluence. This technique offers a simple, yet efficient and attractive approach to produce highly uniform and high aspect ratio silicon nanostructures in the 200–300 nm range.

First-principles simulations were conducted to explore various electronic properties of crystalline SiO2 (α-quartz) under ultrafast laser irradiation. Employing Density Functional Perturbation Theory and the many-body (GW) approximation, we calculated the impact of thermally excited electrons on the electronic specific heat, electron pressure, effective mass, deformation potential, electron-phonon coupling and electron relaxation time of quartz, covering a wide range of electron temperatures, up to 100,000 K. We show that the electron-phonon relaxation time of highly-excited quartz becomes twice faster compared to low-excited states. The deformation potential, which dictates atomic displacement, has a non-monotonic behavior with a well-pronounced minimum at around 16,000 K (2.7 × 1021 cm−3 of excited electrons) where the bond ionicity of the Si-O starts decreasing followed by a cohesion loss at 35,000 K due to the pressure exerted by the excited electrons on the lattice. Consequently, our calculated data, illustrating the evolution of physical parameters, can facilitate simulations of laser-matter interactions and provide predictive insights into the behavior of quartz under experimental conditions. [ABSTRACT FROM AUTHOR]

The origin of high‐spatial‐frequency laser‐induced periodic surface structures, known as HSFLs, has always been a controversial topic. HSFLs of sub‐100 nm periodicity and sub‐20 nm amplitude are generated on tungsten by Ti:sapphire femtosecond laser irradiation under four different processing environments (ambient, air at 10 mbar, Ar at 10 mbar, and vacuum at 10−7 mbar). The topography and subtopography analysis together with two‐temperature model–molecular dynamics simulations reveal that HSFLs formation originates from laser‐induced thermal stresses, implying both surface tension and tensile forces are involved. The experimental observation of subsurface cavitation confirms a hydrodynamics‐based origin for these nanostructures. [ABSTRACT FROM AUTHOR]

Coupling and spatial localization of energy on ultrafast timescales and particularly on the timescale of the excitation pulse in ultrashort laser irradiated dielectric materials are key elements for enabling processing precision beyond the optical limit. Transforming matter on mesoscopic scales facilitates the definition of nanoscale photonic functions in optical glasses. On these timescales, quantum interactions induced by charge non-equilibrium become the main channel for energy uptake and transfer as well as for the material structural change. We apply a first-principles model to determine dynamic distortions of energy bands following the rapid increase in the free-carrier population in an amorphous dielectric excited by an ultrashort laser pulse. Fused silica glass is reproduced using a system of (SiO4)4− tetrahedra, where density functional theory extended to finite-temperature fractional occupation reproduces ground and photoexcited states. Triggered by electronic charge redistribution, a bandgap narrowing of more than 2 eV is shown to occur in fused silica under geometry relaxation. Calculations reveal that the bandgap decrease results from the rearrangement of atoms altering the bonding strength. Despite an atomic movement impacting strongly the structural stability, the observed change of geometry remains limited to 7% of the interatomic distance and occurs on the femtosecond timescale. This structural relaxation is thus expected to take place quasi-instantly following the photon energy flux. Moreover, under intense laser pulse excitation, fused silica loses its stability when an electron temperature of around 2.8 eV is reached. A further increase in the excitation energy leads to the collapse of both the structure and bandgap. [ABSTRACT FROM AUTHOR]

The use of ultrafast cylindrical vector vortex beams in laser–matter interactions permits new ablation features to be harnessed from inhomogeneous distributions of polarization and beam geometry. As a consequence, the ablation process can yield higher ablation efficiency compared with conventional Gaussian beams. These beams prevent surface quality degradation during the ablative processes. When processing stainless steel and titanium, the average surface roughness obtained by deploying the cylindrical vector is up to 94% lower than the Gaussian case, and the processing efficiency is 80% higher. [ABSTRACT FROM AUTHOR]

Evaluating the optical properties of matter under the action of ultrafast light is crucial in modeling laser–surface interaction and interpreting laser processing experiments. We report optimized coefficients for the Drude-Lorentz model describing the permittivity of several transition metals (Cr, W, Ti, Fe, Au, and Ni) under electron-phonon nonequilibrium, with electrons heated up to 30,000 K and the lattice staying cold at 300 K. A Basin-hopping algorithm is used to fit the Drude-Lorentz model to the nonequilibrium permittivity calculated using ab initio methods. The fitting coefficients are provided and can be easily inserted into any calculation requiring the optical response of the metals during ultrafast irradiation. Moreover, our results shed light on the electronic structure modifications and the relative contributions of intraband and interband optical transitions at high electron temperatures corresponding to the laser excitation fluence used for surface nanostructuring. [ABSTRACT FROM AUTHOR]