Simultaneous time-and-space resolved reflectivity and interferometric measurements over a temporal span of 300 ps have been performed in fused silica and sapphire samples excited with 800 nm, 120 fs laser pulses at energies slightly and well above the ablation threshold. The experimental results have been simulated in the frame of a multiple-rate equation model including light propagation. The comparison of the temporal evolution of the reflectivity and the interferometric measurements at 400 nm clearly shows that the two techniques interrogate different material volumes during the course of the process. While the former is sensitive to the evolution of the plasma density in a very thin ablating layer at the surface, the second yields an averaged plasma density over a larger volume. It is shown that self-trapped excitons do not appreciably contribute to carrier relaxation in fused silica at fluences above the ablation threshold, most likely due to Coulomb screening effects at large excited carrier densities. For both materials, at fluences well above the ablation threshold, the maximum measured plasma reflectivity shows a saturation behavior consistent with a scattering rate proportional to the plasma density in this fluence regime. Moreover, for both materials and for pulse energies above the ablation threshold and delays in the few tens of picoseconds range, a simultaneous “low reflectivity” and “low transmission” behavior is observed. Although this behavior has been identified in the past as a signature of femtosecond laser-induced ablation, its origin is alternatively discussed in terms of the optical properties of a material undergoing strong isochoric heating, before having time to substantially expand or exchange energy with the surrounding media.

Periodic structures of alternating amorphous-crystalline fringes have been fabricated in silicon using repetitive femtosecond laser exposure (800 nm wavelength and 120 fs duration). The method is based on the interference of the incident laser light with far- and near-field scattered light, leading to local melting at the interference maxima, as demonstrated by femtosecond microscopy. Exploiting this strategy, lines of highly regular amorphous fringes can be written. The fringes have been characterized in detail using optical microscopy combined modelling, which enables a determination of the three-dimensional shape of individual fringes. 2D micro-Raman spectroscopy reveals that the space between amorphous fringes remains crystalline. We demonstrate that the fringe period can be tuned over a range of 410 nm – 13 µm by changing the angle of incidence and inverting the beam scan direction. Fine control over the lateral dimensions, thickness, surface depression and optical contrast of the fringes is obtained via adjustment of pulse number, fluence and spot size. Large-area, highly homogeneous gratings composed of amorphous fringes with micrometer width and millimeter length can readily be fabricated. The here presented fabrication technique is expected to have applications in the fields of optics, nanoelectronics, and mechatronics and should be applicable to other materials.

Self-assembly (SA) of molecular units to form regular, periodic extended structures is a powerful bottom-up technique for nanopatterning, inspired by nature. SA can be triggered in all classes of solid materials, for instance, by femtosecond laser pulses leading to the formation of laser-induced periodic surface structures (LIPSS) with a period slightly shorter than the laser wavelength. This approach, though, typically involves considerable material ablation, which leads to an unwanted increase of the surface roughness. We present a new strategy to fabricate high-precision nanograting structures in silicon, consisting of alternating amorphous and crystalline lines, with almost no material removal. The strategy can be applied to static irradiation experiments and can be extended into one and two dimensions by scanning the laser beam over the sample surface. We demonstrate that lines and areas with parallel nanofringe patterns can be written by an adequate choice of spot size, repetition rate and scan velocity, keeping a constant effective pulse number (N eff) per area for a given laser wavelength. A deviation from this pulse number leads either to inhomogeneous or ablative structures. Furthermore, we demonstrate that this approach can be used with different laser systems having widely different wavelengths (1030 nm, 800 nm, 400 nm), pulse durations (370 fs, 100 fs) and repetition rates (500 kHz, 100 Hz, single pulse) and that the grating period can also be tuned by changing the angle of laser beam incidence. The grating structures can be erased by irradiation with a single nanosecond laser pulse, triggering recrystallization of the amorphous stripes. Given the large differences in electrical conductivity between the two phases, our structures could find new applications in nanoelectronics.

To overcome the resolution limits in laser processing technologies, it is highly attractive to translate concepts used in advanced optical microscopy. In this prospect, the nonlinear nature of absorption in dielectrics with femtosecond lasers is recurrently taken as a direct advantage in an analogous way to excitation in multiphoton microscopy. However, we establish that no direct benefit in resolution can be expected when laser ablation is observed. We explore widely different nonlinear regimes using ultrashort pulses at different wavelengths (1550 and 515 nm) and target materials of various bandgaps (3.8–8.8 eV). We find in the experiments that the shapes of all ablation features correspond to a one-to-one mapping of the beam contours at a strict threshold intensity. The nonlinearity-independent response shows that the incorporation of extreme UV should provide a direct route to the nanoscale resolutions routinely achieved in lithography.