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We discuss the dynamics of ultrashort pulsed laser excitation in bulk optical silica-based glasses (fused silica and borosilicate BK7) well-above the permanent modification threshold. We indicate subsequent structural and thermomechanical energy relaxation paths that translate into positive and negative refractive index changes, compression and rarefaction zones. If fast electronic decay occurs at low excitation levels in fused silica via self-trapping of excitons, for carrier densities in the vicinity of the critical value at the incident wavelength, persistent long-living absorptive states indicate the achievement of low viscosity matter states manifesting pressure relaxation, rarefaction, void opening and compaction in the neighboring domains. An intermediate ps-long excited carrier dynamics is observed for BK7 in the range corresponding to structural expansion and rarefaction. The amount of excitation and the strength of the subsequent hydrodynamic evolution is critically dependent on the pulse time envelope, indicative of potential optimization schemes.
Given their unique properties, ultrashort laser pulses with durations in the femtosecond to picosecond range currently open new avenues in the field of laser materials processing, resulting in groundbreaking new applications based on laser-induced surface functionalization. This article reviews the usability of temporally distributed energy deposition via double-pulse irradiation in applications based on laser ablation. This includes simple new techniques for surface nanostructuring and improved sensitivities in spectroscopic material analyses.
The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of fused silica and silicon with multiple (NDPS) irradiation sequences consisting of linearly polarized femtosecond laser pulse pairs (pulse duration ~150 fs, central wavelength ~800 nm) is studied experimentally. Nearly equal-energy double-pulse sequences are generated allowing the temporal pulse delay Δt between the cross-polarized individual fs-laser pulses to be varied from -40 ps to +40 ps with a resolution of ~0.2 ps. The surface morphologies of the irradiated surface areas are characterized by means of scanning electron and scanning force microscopy. Particularly for dielectrics in the sub-ps delay range striking differences in the orientation and spatial characteristics of the LIPSS can be observed. For fused silica, a significant decrease of the LIPSS spatial periods from ~790 nm towards ~550 nm is demonstrated for delay changes of less than ~2 ps. In contrast, for silicon under similar irradiation conditions, the LIPSS periods remain constant (~760 nm) for delays up to 40 ps. The results prove the impact of laser-induced electrons in the conduction band of the solid and associated transient changes of the optical properties on fs-LIPSS formation.
In order to address the dynamics and physical mechanisms of LIPSS formation for three different classes of materials (metals, semiconductors, and dielectrics), two-color double-fs-pulse experiments were performed on Titanium, Silicon and Fused Silica. For that purpose a Mach–Zehnder interferometer generated polarization controlled (parallel or cross-polarized) double-pulse sequences at 400 nm and 800 nm wavelength, with inter-pulse delays up to a few picoseconds. Multiple of these two-color double-pulse sequences were collinearly focused by a spherical mirror to the sample surfaces. The fluence of each individual pulse (400 nm and 800 nm) was always kept below its respective ablation threshold and only the joint action of both pulses lead to the formation of LIPSS. Their resulting characteristics (periods, areas) were analyzed by scanning electron microscopy. The periods along with the LIPSS orientation allow a clear identification of the pulse which dominates the energy coupling to the material. For strong absorbing materials (Silicon, Titanium), a wavelength-dependent plasmonic mechanism can explain the delay-dependence of the LIPSS. In contrast, for dielectrics (Fused Silica) the first pulse always dominates the energy deposition and LIPSS orientation, supporting a non-plasmonic formation scenario. For all materials, these two-color experiments confirm the importance of the ultrafast energy deposition stage for LIPSS formation.
The formation of laser-induced periodic surface structures upon irradiation of titanium, silicon, and fused silica with multiple irradiation sequences consisting of parallel polarized Ti:sapphire femtosecond laser pulse pairs (pulse duration 50–150 fs, central wavelength ~800 nm) is studied experimentally. The temporal delay between the individual near-equal energy fs-laser pulses was varied between 0 and 5 ps with a temporal resolution of better than 0.2 ps. The surface morphology of the irradiated surface areas is characterized by means of scanning electron microscopy (SEM). In all materials a decrease of the rippled surface area is observed for increasing delays. The characteristic delay decay scale is quantified and related to material dependent excitation and energy relaxation processes.
Laser-induced periodic surface structures (LIPSS, ripples) are a universal phenomenon that can be observed on almost any material after the irradiation by linearly polarized laser beams, particularly when using ultrashort laser pulses with durations in the picosecond to femtosecond range. During the past few years significantly increasing research activities have been reported in the field of LIPSS, since their generation in a single-step process provides a simple way of nanostructuring and surface functionalization towards the control of optical, mechanical or chemical properties. In this contribution current applications of LIPSS are reviewed, including the colorization of technical surfaces, the control of surface wetting, the tailoring of surface colonization by bacterial biofilms, and the improvement of the tribological performance of nanostructured metal surfaces.
Ablation of single-crystalline (100) indium phosphide wafer surfaces with single 10 fs Ti:sapphire laser pulses in air has been studied by means of complementary cross-sectional transmission electron microscopy, scanning force microscopy, and optical microscopy. A local protrusion of ~70 nm height is generated within the ablation craters for fluences exceeding 0.78 J/cm². This morphological feature has been studied in detail, revealing the material structure of the laser-affected zone and its spatial extent. The resolidified layer (60-200 nm thick) consists of polycrystalline grains (5-15 nm diameter) and is covered by an ~10 nm thick amorphous top layer. Interestingly, the sharp boundary of the solidified layer to the unaffected crystal underneath exhibits a Gaussian-like shape and does not follow the shape of the surface topography. Evidence is presented that the central crater protrusion is formed by near-surface optical breakdown, and that the absorption in the material transiently changes during the femtosecond-laser pulse.