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Modern life and global communication would not be possible without technologically tailored thin films; they are omnipresent in daily life applications. In most cases, the films are deposited entirely at the carrying substrates in a specific processing step of the device or sample. In some cases, however, removal or modification must be performed locally, i.e., site-controlled and material selective through an additional laser processing step. For that ultrashort laser pulses with durations in the femtosecond and picosecond range can provide unique advantages and capabilities in industrially scalable schemes. This article reviews the current state of the research and corresponding industrial transfer related to the structuring of thin films by ultrashort pulsed lasers. It focuses on the pertinent historic developments, reveals the relevant physical and chemical effects, explores the ultimate limits, and discusses selected industrial and scientific applications.
Micro- and nanostructuring with laser-induced periodic surface structures (LIPSS) has been demonstrated to be feasible in a wide variety of materials including metals, semiconductors and dielectrics. Suitable processing regimes for flat, curved and complex surfaces have been identified for many materials, allowing the generation of diverse applications in fields such as optics, tribology and medicine, to name a few. A common side effect when producing such structures in air environment is the formation of a thin surface oxide layer in the laser irradiated areas. Previous studies have shown that oxidation plays an important role in the tribological performance for which the structures where created, and very recently it has been shown that the laser-induced oxide graded layers may contribute to the formation of a new type of embedded low-spatial frequency LIPSS (LSFL) with annomalous orientation parallel to the laser polarization, in addition to the appearance of the well-known high-spatial frequency LIPSS (HSFL) at the surface. In this contribution, we explore this effect experimentally for chromium nitride (CrN) irradiated with femtosecond laser pulses and compare the findings to finite-difference time-domain (FDTD) simulations of the intensity distributions at different depth positions.
The redeposited material (debris) resulting from ablation of a potassium–magnesium silicate glass upon scanning femtosecond laser pulse irradiation (130 fs, 800 nm) in air environment is investigated by means of three complementary surface analytical methods. Changes in the electronic band structure of the glass constituent Magnesium (Mg) were identified by X-ray Absorption Near Edge Structure spectroscopy (XANES) using synchrotron radiation. An up-shift of ≈0.8 eV of a specific Magnesium Κ-edge absorption peak in the spectrum of the redeposited material along with a significant change in its leading edge position was detected. In contrast, the surface left after laser ablation exhibits a downshift of the peak position by ≈0.9 eV. Both observations may be related to a change of the Mg coordinative state of the laser modified/redeposited glass material. The presence of carbon in the debris is revealed by micro Raman spectroscopy (µ-RS) and was confirmed by energy dispersive X-ray spectroscopy (EDX). These observations are attributed to structural changes and chemical reactions taking place during the ablation process.
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.
The irradiation of single-crystalline indium phosphide (c-InP) by Ti:sapphire femtosecond laser pulses (130 fs, 800 nm) in air is studied by means of in-situ time resolved reflectivity measurements [fs-time-resolved microscopy (100 fs-10 ns) and point probing analysis (ns - µs)] and by complementary ex-situ surface analytical methods (Micro Raman Spectroscopy, Scanning Force, and Optical Microscopy). The dynamics of melting, ablation, and optical breakdown as well as structural changes resulting from rapid solidification are investigated in detail. Different laser-induced surface morphologies are characterized and discussed on the basis of recent ablation and optical breakdown models.
The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of silicon wafer surfaces by linearly polarized Ti:sapphire femtosecond laser pulses (pulse duration 130 fs, central wavelength 800 nm) is studied experimentally and theoretically. In the experiments, so-called low-spatial frequency LIPSS (LSFL) were found with periods smaller than the laser wavelength and an orientation perpendicular to the polarization. The experimental results are analyzed by means of a new theoretical approach, which combines the widely accepted LIPSS theory of Sipe et al. with a Drude model, in order to account for transient (intra-pulse) changes of the optical properties of the irradiated materials. It is found that the LSFL formation is caused by the excitation of surface plasmon polaritons, SPPs, once the initially semiconducting material turns to a metallic state upon formation of a dense free-electron-plasma in the material and the subsequent interference between its electrical field with that of the incident laser beam resulting in a spatially modulated energy deposition at the surface. Moreover, the influence of the laser-excited carrier density and the role of the feedback upon the multi-pulse irradiation and its relation to the excitation of SPP in a grating-like surface structure is discussed.
The dynamics of the formation of laser-induced periodic surface structures (LIPSS) on fused silica upon irradiation with linearly polarized fs-laser pulses (50 fs pulse duration) is studied by cross-polarized two-color double-fs-pulse experiments. In order to analyze the relevance of temporally distributed energy deposition in the early stage of LIPSS formation, a Mach-Zehnder interferometer was used for generating multiple double-pulse sequences at two different wavelengths (400 and 800 nm). The inter-pulse delay between the individual cross-polarized pulses of each sequence was systematically varied in the sub-ps range and the resulting LIPSS morphologies were characterized by scanning electron microscopy. It is found that the polarization of the first laser pulse arriving to the surface determines the orientation and the periodicity of the LIPSS. These two-color experiments further confirm the importance of the ultrafast energy deposition to the silica surface for LIPSS formation, particularly by the first laser pulse of each sequence. The second laser pulse subsequently reinforces the previously seeded spatial LIPSS characteristics (period, orientation).
Herein, Ti6Al4V alloy is surface modified by femtosecond laser ablation. The microstructure image obtained by secondary electron microscopy reveals a combination of micrometer spikes or cones superimposed by nanoripples (laser‐induced periodic surface structures). To make the surface hydrophilic, anodization is performed resulting in further smoothness of microstructure and a final thickness of 35 ± 4 nm is estimated for oxide produced after anodization at 10 V (scan rate = 0.1 V s−1) versus standard hydrogen electrode. The obtained electrochemically active surface area (ECSA) is approximately 8 times larger compared with flat mirror polished Ti6Al4V surface. Combined chemical analysis by Pourbaix diagram and X‐ray photoelectron spectroscopy (XPS) analyses reveal that titanium and aluminum are passivating into TiO2 and Al2O3, but the dissolution of aluminum in the form of solvated ion is inevitable. Finally, cell seeding experiments on anodized and laser‐treated titanium alloy samples show that the growth of murine fibroblast cells is significantly suppressed due to unique surface texture of the laser‐treated and anodized titanium alloy sample.
Sub-100-nm laser-induced periodic surface structures (LIPSS) were processed on bulk titanium (Ti) surfaces by femtosecond laser pulse irradiation in air (30 fs pulse duration, 790 nm wavelength). The laser peak fluence, the spatial spot overlap, and the number of overscans were optimized in a sample-scanning geometry in order to obtain large surface areas (5 mm × 5 mm) covered homogeneously by the LIPSS. The laser-processed regions were characterized by optical microscopy (OM), white light interference microscopy (WLIM) and scanning electron microscopy (SEM). The friction coefficient of the nanostructured surfaces was tested during 1000 cycles under reciprocal sliding conditions (1 Hz, 1.0 N normal load) against a 10-mm diameter ball of hardened 100Cr6 steel, both in paraffin oil and in engine oil used as lubricants. Subsequently, the corresponding wear tracks were qualified by OM, SEM, and energy dispersive X-ray analyses (EDX). The results of the tribological tests are discussed and compared to that obtained for near wavelength-sized fs-LIPSS, processed under somewhat different irradiation conditions. Some constraints for a beneficial effect of LIPSS on the tribological performance are provided.