The unique characteristics of ultrafast lasers, such as picosecond and femtosecond lasers, have opened up new avenues in materials processing that employ ultrashort pulse widths and extremely high peak intensities. Thus, ultrafast lasers are currently used widely for both fundamental research and practical applications. This review describes the characteristics of ultrafast laser processing and the recent advancements and applications of both surface and volume processing. Surface processing includes micromachining, micro- and nanostructuring, and nanoablation, while volume processing includes two-photon polymerization and three-dimensional (3D) processing within transparent materials. Commercial and industrial applications of ultrafast laser processing are also introduced, and a summary of the technology with future outlooks are also given. Scientists in Asia have reviewed the role of ultrafast lasers in materials processing. Koji Sugioka from RIKEN in Japan and Ya Cheng from the Shanghai Institute of Optics and Fine Mechanics in China describe how femtosecond and picosecond lasers can be used to perform useful tasks in both surface and volume processing. Such lasers can cut, drill and ablate a variety of materials with high precision, including metals, semiconductors, ceramics and glasses. They can also polymerize organic materials that contain a suitable photosensitizer and can three-dimensionally process inside transparent materials such as glass, and are already being used to fabricate medical stents, repair photomasks, drill ink-jet nozzles and pattern solar cells. The researchers also explain the characteristics of such lasers and the interaction of ultrashort, intense pulses of light with matter.

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Ultrafast lasers—reliable tools for advanced materials processing

This paper reviews a new field of direct femtosecond laser surface nano/microstructuring and its applications. Over the past few years, direct femtosecond laser surface processing has distinguished itself from other conventional laser ablation methods and become one of the best ways to create surface structures at nano- and micro-scales on metals and semiconductors due to its flexibility, simplicity, and controllability in creating various types of nano/microstructures that are suitable for a wide range of applications. Significant advancements were made recently in applying this technique to altering optical properties of metals and semiconductors. As a result, highly absorptive metals and semiconductors were created, dubbed as the “black metals” and “black silicon”. Furthermore, various colors other than black have been created through structural coloring on metals. Direct femtosecond laser processing is also capable of producing novel materials with wetting properties ranging from superhydrophilic to superhydrophobic. In the extreme case, superwicking materials were created that can make liquids run vertically uphill against the gravity over an extended surface area. Though impressive scientific achievements have been made so far, direct femtosecond laser processing is still a young research field and many exciting findings are expected to emerge on its horizon.

Direct femtosecond laser surface nano/microstructuring and its applications

We show that short-pulse laser-induced classical ripples on dielectrics, semiconductors, and conductors exhibit a prominent "non-classical" characteristic-in normal incidence the periods are definitely smaller than laser wavelengths, which indicates that the simplified scattering model should be revised. Taking into account the surface plasmons (SPs), we consider that the ripples result from the initial direct SP-laser interference and the subsequent grating-assisted SP-laser coupling. With the model, the period-decreasing phenomenon originates in the admixture of the field-distribution effect and the grating-coupling effect. Further, we propose an approach for obtaining the dielectric constant, electron density, and electron collision time of the high-excited surface. With the derived parameters, the numerical simulations are in good agreement with the experimental results. On the other hand, our results confirm that the surface irradiated by short-pulse laser with damage-threshold fluence should behave metallic, no matter for metal, semiconductor, or dielectric, and the short-pulse laser-induced subwavelength structures should be ascribed to a phenomenon of nano-optics.

Origin of laser-induced near-subwavelength ripples: interference between surface plasmons and incident laser

The formation of laser-induced periodic surface structures (LIPSS) in different materials (metals, semiconductors, and dielectrics) upon irradiation with linearly polarized fs-laser pulses (τ ∼ 30–150 fs, λ ∼ 800 nm) in air environment is studied experimentally and theoretically. In metals, predominantly low-spatial-frequency-LIPSS with periods close to the laser wavelength λ are observed perpendicular to the polarization. Under specific irradiation conditions, high-spatial-frequency-LIPSS with sub-100-nm spatial periods (∼λ/10) can be generated. For semiconductors, the impact of transient changes of the optical properties to the LIPSS periods is analyzed theoretically and experimentally. In dielectrics, the importance of transient excitation stages in the LIPSS formation is demonstrated experimentally using (multiple) double-fs-laser-pulse irradiation sequences. A characteristic decrease of the LIPSS periods is observed for double-pulse delays of less than 2 ps.

Femtosecond laser-induced periodic surface structures

Laser-induced periodic surface structures (LIPSS, ripples) are a universal phenomenon and can be generated on almost any material upon irradiation with linearly polarized radiation. With the availability of ultrashort laser pulses, LIPSS have gained an increasing attraction during the past decade, since these structures can be generated in a simple single-step process, which allows a surface nanostructuring for tailoring optical, mechanical, and chemical surface properties. In this study, the current state in the field of LIPSS is reviewed. Their formation mechanisms are analyzed in ultrafast time-resolved scattering, diffraction, and polarization constrained double-pulse experiments. These experiments allow us to address the question whether the LIPSS are seeded via ultrafast energy deposition mechanisms acting during the absorption of optical radiation or via self-organization after the irradiation process. Relevant control parameters of LIPSS are identified, and technological applications featuring surface functionalization in the fields of optics, fluidics, medicine, and tribology are discussed.

Laser-Induced Periodic Surface Structures— A Scientific Evergreen

Ripples revisited: non-classical morphology at the bottom of femtosecond laser ablation craters in transparent dielectrics

Surface structures and structural transformations are investigated upon femtosecond laser ablation (800 nm, 120 fs) from crystalline silicon (100) targets placed under ultra-high vacuum. After repetitive illumination with several thousand laser pulses at intensities below the single shot damage threshold, at normal incidence, the crater morphology indicates the development of periodic structures at the crater bottom, with the orientation depending on the laser beam polarization. Periods of 200 nm and 600–700 nm, respectively, are shorter than the laser wavelength and appear as a result of surface instability. The ablation dynamics monitored by time-of-flight mass spectrometry shows the emission of positive silicon ions and clusters with kinetic energies of about 7 eV. Raman spectroscopy reveals phase transformations in the irradiated spot from Si-I to the polymorphs Si-III, Si-IV, Si-XII, and amorphous silicon as well as a stable, uncommon phase of hexagonal Si-wurzite.

Sub–damage–threshold femtosecond laser ablation from crystalline Si: surface nanostructures and phase transformation

Surface patterning on insulators upon femtosecond laser ablation

Self-organized pattern formation upon femtosecond laser ablation by circularly polarized light

In self-organized nanostructure formation upon femtosecond laser ablation, the laser polarization is an important control parameter. Experiments on fluoride crystals, using circular and elliptical polarization, study this influence in more detail. For circular polarization, spherical nanoparticles of about 100 nm diameter are formed. With increasing ellipticity, longer and longer ordered chains and linear structures are generated, oriented perpendicular to the long axis of the polarization ellipse. A similar effect occurs when, for circular polarization, the angle of incidence is varied from normal to 45°: the s-component of the incident field, not attenuated by the projection, determines length and orientation of the ordered ripples. However, surface defects like scratches exert an even stronger influence on the ripples orientation than the polarization, resulting in curved structures bending from polarization-controlled to defect-controlled orientation. Since the structure formation takes place only long after the end of the laser pulse, a certain electrical field memorizer is required to account for this polarization dependence. A promising approach assumes directional atomic surface diffusion anisotropies, arising, e.g. from plasmon-coupled metal–colloid arrays.

Florenta Costache

Papers

Ripples revisited: non-classical morphology at the bottom of femtosecond laser ablation craters in transparent dielectrics

Sub–damage–threshold femtosecond laser ablation from crystalline Si: surface nanostructures and phase transformation

Surface patterning on insulators upon femtosecond laser ablation

Self-organized pattern formation upon femtosecond laser ablation by circularly polarized light

Femtosecond laser induced nanostructure formation: self-organization control parameters