High Spatial Frequency LIPSS Research Articles

Energy–dependent femtosecond LIPSS on germanium and application in explosives sensing

Abstract In this study, we fabricated laser-induced periodic surface structures (LIPSS) on a germanium surface through laser ablation in air using axicon and femtosecond (fs) pulses. This novel approach permitted the nanoscale material processing outcome refinement via an fs Bessel beam. Our investigations aimed at systematically understanding the formation of periodic structures under various experimental conditions, such as (i) different pulse energies ranging from 50 µJ to 1000 µJ at a constant scan speed and (ii) constant energy with different scan speeds (0.1–3 mm s−1). By adjusting the fluences and scan speeds, we were able to identify the parametric space and alter the periodicity of the low-spatial frequency LIPSS and high-spatial frequency LIPSS on germanium, which were analyzed using field emission scanning electron microscopy. An optimal LIPSS formation over a large area of germanium was achieved at an input energy of 250 µJ and a scan speed of 0.75 mm s−1. Additionally, we measured the contact angles of the Ge nanostructures (GeNSs) to demonstrate their hydrophobic nature and non-wetting properties, providing insights into the behavior of LIPSS. Subsequently, the GeNSs were coated with a ∼15 nm thick gold (Au) film using a thermal deposition method. Utilizing these, the surface-enhanced Raman spectroscopy (SERS) technique detected diverse analytes, such as tetryl (an explosive) at a concentration of 50 µM and thiram (a pesticide) at 500 nM. The SERS enhancement factors for tetryl and thiram molecules on GeNSs coated with a 15 nm-thick Au layer were determined to be 2.5 × 104 and 4.2 × 105, respectively.

Point defect distributions in ultrafast laser-induced periodic surface structures on β-Ga2O3

β-Ga2O3 has received widespread attention due to its ultrawide bandgap, which potentially permits applications in extreme conditions. Ultrafast laser irradiation of β-Ga2O3 provides a means for exploring the response of the material under such conditions, which could result in the generation of point defects as well as a localized modification of structural features that could yield properties that differ from the pristine surface. However, an understanding of defects generated by femtosecond laser irradiation in the vicinity of laser-induced periodic surface structures (LIPSS) remains to be explored. We correlate topographic features with optical and electronic properties by combining near-nm scale resolution cathodoluminescence with Kelvin probe force microscopy. Defects are found to correlate with crystalline order and near-surface morphology, as well as changes in work function. They are also suggested to be closely related to the formation of high spatial frequency LIPSS. These results suggest a need for precise tuning of laser irradiation conditions as well as possible post-processing to control defects in future Ga2O3 devices.

Fabrication of grooves on 4H–SiC using femtosecond laser vector beam

Femtosecond lasers are widely acknowledged for their capability to groove and generate laser-induced periodic surface structures (LIPSS) on various materials. LIPSS structures include LSFL (low spatial frequency LIPSS) and HSFL (high spatial frequency LIPSS). In this study, a segmented waveplate (SWP) was used to transform a linearly polarized femtosecond laser Gaussian beam with a wavelength of 515 nm into a vector beam with a donut-shaped energy peak distribution and polarization of azimuthal and radial. Grooving was conducted on three different SiC surface conditions: polished and pre-processed (LSFL and HSFL), using linear, azimuthal, and radial polarization. This study investigated the differences in microstructure morphology and compared the ablation depths of the grooves. It was found that grooving on pre-processed LSFL 4H–SiC surfaces resulted in grooves with higher ablation depths than those produced on polished surfaces. Additionally, using azimuthal polarization on the HSFL surface could create fine HSFL structures (with a period of approximately 100 nm) between the initial periodic structures (with a period of approximately 250 nm) formed during the pre-processing.

Efficient fabrication of high-quality hybrid periodic nanostructures on 4H-SiC using a single-step vector femtosecond laser processing

Femtosecond lasers are widely recognized for generating laser-induced periodic surface structures (LIPSS) on various materials. Moreover, the homogeneous low spatial frequency LIPSS (H-LSFL) can be achieved by employing linear scanning with polarized femtosecond laser pulses and precise control of parameters, such as fluence and scanning speed. Unlike traditional LSFLs, these H-LSFLs are characterized by uniform structures. This study demonstrates the high-precision fabrication of hybrid periodic nanostructures, specifically H-LSFL with vertically aligned HSFL (high-spatial frequency LIPSS) on 4H-SiC using azimuthally polarized femtosecond laser beams. The experimental results revealed that the rapid fabrication of two parallel line patterns featuring hybrid periodic nanostructures can be achieved in a single scanning pass. Furthermore, a beam expander was employed to reduce the laser’s focal spot size, increasing the distribution of HSFL concerning H-LSFL as the distance between line segments decreased.

Investigating the transition from high to low spatial frequency periodic nanoripples on TiO2 (0 0 1) oriented surface upon irradiation with UV-femtosecond pulses

The formation of laser-induced periodic surface structures (LIPSS) on a TiO2 (001) oriented surface upon irradiation with UV-fs laser pulses was analyzed. Two systems of low spatial frequency LIPSS (LSFL) perpendicular to the direction of laser polarization are observed after N = 5 laser pulses. One was developed on the edges of the crater created by the first laser pulse, while the other appeared in the center of crater and spread towards the edges. When N was greater than 10, the two LIPSS systems merge. Both LSFL systems have a spatial period of approximately 200 nm and are due to the coherent superposition of surface waves scattered on inhomogeneities of a transient metallic surface. However they differ by the type of defects involved in the excitation process of surface waves. While a pronounced and localized rim triggered LSFL on the edge of the laser spot, LSFL in the central part nucleated at the shallow high spatial frequency LIPSS (HSFL), which are parallel to the laser polarization. A mechanism is proposed to explain the role of the HSFL in the formation of LSFL. Numerical simulations of the absorbed laser power density support the evolution from HSFL to LSFL as the number of laser pulses increased.

Polarization-Dependent Anisotropy of LIPSSs' Morphology Evolution on a Single-Crystal Silicon Surface.

Utilizing the principle of laser-induced periodic surface structures (LIPSSs), this research delves into the morphological evolution of single-crystal silicon surfaces irradiated by a near-infrared picosecond laser through a scanning mode. With the increase in laser energy density, the nanostructure morphology on single-crystal silicon surfaces induced by incident lasers with different polarization directions sequentially produces high spatial-frequency LIPSSs (HSFLs) with a period of 220 nm ± 10 nm parallel to the laser polarization, low spatial-frequency LIPSSs (LSFLs) with a period of 770 nm ± 85 nm perpendicular to the direction of the polarization, and groove structures. Furthermore, by varying the angle between the laser polarization and the scanning direction, the study examined the combined anisotropic effects of the laser polarization scanning direction angle and the laser polarization crystal orientation angle on the genesis of LIPSSs on single-crystal silicon (100) surfaces. The experiments revealed polarization-related anisotropic characteristics in the morphology of HSFLs. It was found that when the polarization angle approached 45°, the regularity of the LSFLs deteriorated, the modification width decreased, and the periodicity increased. This is critical for the precise control of the LSFLs' morphology.

Investigating Laser-Induced Periodic Surface Structures (LIPSS) Formation in Silicon and Their Impact on Surface-Enhanced Raman Spectroscopy (SERS)

Laser-induced periodic surface structures (LIPSS) have gained significant attention due to their ability to modify the surface morphology of materials at the micro-nanoscale and show great promise for surface functionalization applications. In this study, we specifically investigate the formation of LIPSS in silicon substrates and explore their impact on surface-enhanced Raman spectroscopy (SERS) applications. This study reveals a stepwise progression of LIPSS formation in silicon, involving three distinct stages of LIPSS: (1) integrated low-spatial-frequency LIPSS (LSFL) and high-spatial-frequency LIPSS (HSFL), (2) principally LSFL and, (3) LSFL at the edge of the irradiated spot, elucidating the complex interplay between laser fluence, pulse number, and resulting surface morphology. Furthermore, from an application standpoint, these high-quality multi-scale periodic patterns lead to the next step of texturing the entire silicon surface with homogeneous LIPSS for SERS application. The potential of LIPSS-fabricated silicon substrates for enhancing SERS performance is investigated using thiophenol as a test molecule. The results indicate that the Au-coated combination of LSFL and HSFL substrates showcased the highest enhancement factor (EF) of 1.38×106. This pronounced enhancement is attributed to the synergistic effects of localized surface plasmon resonance (LSPR) and surface plasmon polaritons (SPPs), intricately linked to HSFL and LSFL characteristics. These findings contribute to our understanding of LIPSS formation in silicon and their applications in surface functionalization and SERS, paving the way for sensing platforms.

Investigation of Laser-Induced Surface Structures (LIPSS) on quartz and evaluation of their influence on material wettability

We report here on a study of the generation of Laser-Induced Periodic Surface Structures (LIPSS) on quartz upon irradiation with linearly polarized femto-second laser pulses (pulse duration τ = 200 fs and central wavelength λ = 1030 nm). Two different regimes of LIPSS were observed, Low-Spatial-Frequency-LIPSS (LSFL) and High-Spatial-Frequency-LIPSS (HSFL), characterized by different spatial periods and orientations. The formation of these two types of structures was investigated by varying the laser fluence, the number of laser pulses and the laser repetition rate. Once established how these parameters affect the generation of LIPSS, extended HSFL patterns (25 × 25 mm2) were realized, and their wettability was compared to that of pristine quartz. Contact angle measurements showed that HSFL textured quartz exhibits a super-hydrophilic behaviour, with a measured contact angle equal to 7.6°, with respect to pristine quartz which results simply hydrophilic and shows a contact angle equal to 41.2°.

Formation and modulation of multi-pulse femtosecond laser-induced periodic surface structures by electromagnetic and partial differential equation simulations.

In order to demonstrate the formation of laser-induced periodic surface structures (LIPSS), simulations were performed to investigate the effect of multiple femtosecond laser pulses with different laser energy densities on a Ti6Al4V surface. In this work, a set of partial differential equations calculating the electron and lattice temperature variations, followed by coupling with an electric field, is used to analyze the evolution of the periodic surface structure induced by the interaction of the femtosecond laser with the material. As the number of pulses increases, the surface structure of the material changes from none to produce LIPSS structure and from low spatial frequency LIPSS (LSFL) structure to high spatial frequency LIPSS (HSFL) structure. In order to compare the results, single-point laser scanning ablation experiments were carried out at femtosecond laser energy. The experimental results are consistent with the simulation results.

Direct Femtosecond Laser Processing for Generating High Spatial Frequency LIPSS (HSFL) on Borosilicate Glasses with Large-Area Coverage

Large-area nanostructuring of glasses using intense laser beams is a challenging task due to the material’s extreme non-linear absorption of laser energy. Precise optimization of the process parameters is essential for fabricating nanostructures with large-area coverage. In this study, we report the findings on creating high-spatial-frequency LIPSS (HSFL) on borosilicate glass through direct laser writing, using a femtosecond laser with a wavelength λ = 800 nm, pulse duration τ = 35 fs, and repetition frequency frep = 1 kHz. We measured the single-pulse ablation threshold and incubation factor of Borosilicate glasses to achieve high-precision control of the large-area surface structuring. Single-spot experiments indicated that, when there was higher fluence and a larger number of irradiated laser pulses, a melt formation inside the irradiated area limited the uniformity of LIPSS formation. Additionally, the orientation of the scan axis with the laser beam polarization was found to significantly influence the uniformity of LIPSS generated along the scan line, with more redeposition and melt formation when the scan axis was perpendicular to the laser beam polarization. For large-area processing, the borosilicate glass surface was scanned line-by-line by the laser beam, with a scan orientation parallel to the polarization of the laser. The optical characterization revealed that the transmittance and reflectance of the borosilicate glass decreased significantly after processing. Additionally, the surface’s wettability changed from hydrophilic to super-hydrophilic after processing. These chemical contamination-free and uniformly distributed structures have potential applications in optics, microfluidics, photovoltaics, and biomaterials.

Formation of Laser-Induced Periodic Surface Structures on Reaction-Bonded Silicon Carbide by Femtosecond Pulsed Laser Irradiation

Reaction-bonded silicon carbide (RB-SiC) is an excellent engineering material with high hardness, stiffness, and resistance to chemical wear. However, its widespread use is hindered due to the properties mentioned above, making it difficult to machine functional surface structures through mechanical and chemical methods. This study investigated the fundamental characteristics of laser-induced periodic surface structures (LIPSSs) on RB-SiC via femtosecond pulsed laser irradiation at a wavelength of 1028 nm. Low-spatial-frequency LIPSS (LSFL) and high-spatial-frequency LIPSS (HSFL) formed on the surface along directions perpendicular to the laser polarization. SiC grains surrounded by a large amount of Si show a reduced threshold for LIPSS formation. By varying laser fluence and scanning speed, HSFL–LSFL hybrid structures were generated on the SiC grains. Transmission electron microscopy observations and Raman spectroscopy were carried out to understand the formation mechanism of the hybrid LIPSS. A possible mechanism based on the generation of multiple surface electromagnetic waves due to the nonlinear response of SiC was proposed to explain the hybrid structure formation. Furthermore, the direction of laser scanning with respect to laser polarization affects the uniformity of the generated LIPSS.

Study on the Origin and Evolution of Femtosecond Laser-Induced Surface Structures: LIPSS, Quasi-Periodic Grooves, and Aperiodic Micro-Ridges.

We investigate the evolution mechanisms of the laser-induced periodic surface structures (LIPSS) and quasi-periodic grooves that are formed on the surface of monocrystalline silicon (mono-Si) when exposed to femtosecond laser radiation of different pulse duration, state of polarization, and fluence. The conditions required for producing LIPSS-free complex micro-ridge patterns are elaborated. The LIPSS evolution mechanism is explained in terms of scattering/interference-based phenomena. To establish the basis for our interpretation, single femtosecond pulses of different pulse durations are irradiated on mono-Si. The absence/appearance of LIPSS rudiments is explained in the context of spectral bandwidth and the associated effects on the intensity of the central wavelength. Shorter fs pulses of a wider bandwidth are employed to induce LIPSS-free micro-ridge patterns. It is demonstrated that the resultant micro-ridge patterns depend on the laser fluence distribution and can be manipulated through laser polarization. The curved morphology of LIPSS rudiments and the evolution mechanism of low- and high-spatial frequency LIPSS, i.e., LSFL and HSFL, are discussed. Finally, it is demonstrated that the consolidated quasi-periodic grooves result from HSFL welding together groups of LSFL. Although our findings are based on fs laser interaction with mono-Si, the results can also be applied to many other materials.

Laser ablation of RB-SiC composite by femtosecond laser irradiation

Reaction-bonded silicon carbide composites (RB-SiC), consisting of SiC grains and Si matrix, have a complex ablation mechanism as two-phase composites under femtosecond laser irradiation. The ablation threshold of RB-SiC was calculated, which decreases (from 1.01 J/cm2 to 0.56 J/cm2) with increasing pulse number N and finally stabilized. At low fluence (F/Fth ≤ 5) and a low number of pulses, photochemical ablation dominates. For a higher number of pulses and high fluence (5 <F/Fth ≤ 50), photothermal ablation dominates with photochemical ablation. The results show that structures such as pits, convex, and holes exist on the surface of Crater I, while Laser-induced Periodic Surface Structures (LIPSS), and condensation structures exist on the surface of Crater II. In both types of ablation craters, the SiC grain surface produces the Low Spatial Frequency LIPSS (LSFL) with a period of about 900 nm and the High Spatial Frequency LIPSS (HSFL) with a period of about 300 nm. Based on the surface morphology, microstructure, and physical phase analysis of the ablation craters, a preliminary model of the removal mechanism of the ablation craters by femtosecond laser irradiation was established. These findings are expected to provide theoretical and experimental support for the precision processing of RB-SiC by femtosecond laser.

Femtosecond laser-induced periodic surface structures on diamond-like nanocomposite films

We study the formation of laser-induced periodic surface structures (LIPSS) on diamond-like nanocomposite (DLN) a-C:H:Si:O films and titanium-doped DLN films during femtosecond (fs) laser ablation processing with linearly-polarized beams of IR and visible fs-lasers (wavelengths 1030 nm and 515 nm, pulse duration 320 fs, pulse repetition rates 100 kHz-2 MHz, scanning beam velocity 0.04–0.4 m/s). The studies are focused on (i) comparison of high spatial frequency LIPSS (HSFL) and low spatial frequency LIPSS (LSFL) formed on DLN and Ti-DLN films by IR fs-laser processing, (ii) effects of the pulse repetition rate on the parameters of LIPSS formed on the DLN and Ti-DLN films, (iii) Raman spectroscopy analysis of the LIPSS-structured films with application for ultrathin surface graphitization, and (iv) relationship between the fs-laser-induced surface graphitization and LIPSS formation on the films. A variety of the HSFL and LSFL have been produced on the surface of DLN and Ti-DLN films, with all the LIPSS being oriented perpendicular to the beam polarization direction. The HSFL periods are varied from ~80 to 240 nm and the LSFL periods are varied from 355 to 840 nm, depending on the fs-laser irradiation conditions (wavelength, fluence, pulse repetition rate) and films properties. Various plasmonic effects such as the superposition of the HSFL and LSFL and emergence of very unusual sinusoid-like structures on the DLN and Ti-DLN films are presented and discussed. • LIPSS fabrication on DLN and Ti-DLN films with IR and visible femtosecond lasers • Effect of surface graphitization on HSFL and LSFL formation thresholds • Raman analysis of ultrathin surface graphitization on LIPSS-structured DLN films • Influence of pulse repetition rate on fs-laser ablation and LIPSS parameters • Plasmonic effects in the fs-LIPSS formation on diamond-like nanocomposite films

Surface birefringence in FTO thin film fabricated by ultrafast laser

Ultrafast laser-induced periodic surface structures (LIPSSs) have been studied intensely in the last two decades, which have become a useful method for surface nanostructures and are widely used to tune surface properties. This paper reported the fabrication of high-spatial-frequency LIPSSs (HSFLs) on FTO film induced by 1,030[Formula: see text]nm femtosecond laser. The morphology, duty cycle and birefringence effects of HSFLs were studied in detail by changing the laser fluence and scanning speed. Clear and uniform HSFLs were formed over the entire ablated area when the laser fluence and scanning speed were 89[Formula: see text]mJ/cm2 and 0.01[Formula: see text]mm/s, respectively. The duty cycle of the HSFL was measured to be as high as 0.36, and the thickness of the HSFL layer was found to be in the range of 409–546[Formula: see text]nm. The phase retardation of the FTO film with HSFLs could reach up to 96[Formula: see text]nm and could be used as an optical attenuator with a tunable range of 71–100% for 532[Formula: see text]nm linear polarized light.

Regular Periodic Surface Structures on Indium Tin Oxide Film Efficiently Fabricated by Femtosecond Laser Direct Writing with a Cylindrical Lens.

Regular laser-induced periodic surface structures (LIPSS) were efficiently fabricated on indium tin oxide (ITO) films by femtosecond laser direct writing with a cylindrical lens. It was found that randomly distributed nanoparticles and high spatial frequency LIPSSs (HSFL) formed on the surface after a small number of cumulative incident laser pulses per spot, and regular low spatial frequency LIPSSs (LSFL) appeared when more laser pulses accumulated. The mechanism of the transition was studied by real-time absorptance measurement and theoretical simulation. Results show that the interference between incident laser and surface plasmon polaritons (SPPs) excited by random surface scatterers facilitates the formation of prototype LSFLs, which in turn enhances light absorption and SPP excitation following laser pulses. The effects of scanning velocity and laser fluence on LSFL quality were discussed in detail. Moreover, large-area extremely regular LSFL with a diameter of 30 mm were efficiently fabricated on an ITO film by femtosecond laser direct writing with the cylindrical lens. The fabricated LSFLs on the ITO film demonstrate vivid structural color. During LSFL processing, the decrease of ITO film thickness leads to the increase of near-infrared optical transmittance.

Sub-Threshold Fabrication of Laser-Induced Periodic Surface Structures on Diamond-like Nanocomposite Films with IR Femtosecond Pulses.

In the paper, we study the formation of laser-induced periodic surface structures (LIPSS) on diamond-like nanocomposite (DLN) a-C:H:Si:O films during nanoscale ablation processing at low fluences—below the single-pulse graphitization and spallation thresholds—using an IR fs-laser (wavelength 1030 nm, pulse duration 320 fs, pulse repetition rate 100 kHz, scanning beam velocity 0.04–0.08 m/s). The studies are focused on microscopic analysis of the nanostructured DLN film surface at different stages of LIPSS formation and numerical modeling of surface plasmon polaritons in a thin graphitized surface layer. Important findings are concerned with (i) sub-threshold fabrication of high spatial frequency LIPSS (HSFL) and low spatial frequency LIPSS (LSFL) under negligible surface graphitization of hard DLN films, (ii) transition from the HSFL (periods of 140 ± 30 and 230 ± 40 nm) to LSFL (period of 830–900 nm) within a narrow fluence range of 0.21–0.32 J/cm2, (iii) visualization of equi-field lines by ablated nanoparticles at an initial stage of the LIPSS formation, providing proof of larger electric fields in the valleys and weaker fields at the ridges of a growing surface grating, (iv) influence of the thickness of a laser-excited glassy carbon (GC) layer on the period of surface plasmon polaritons excited in a three-layer system “air/GC layer/DLN film”.

Femtosecond laser two-beam interference applied to 4H-SiC surface hierarchical micro-nano structure fabrication

This study used the ultrashort pulsed direct laser interference patterning (USP-DLIP) and a single Gaussian beam process to generate the surface structures on 4H-SiC. The diffractive optical element separated the single beam into two beams and then interfered on the 4H-SiC surface for material processing. The experimental results obtained by USP-DLIP and a single Gaussian beam process were compared. USP-DLIP uses the superposition of two femtosecond laser beams to re-adjust the laser energy distribution. It is characterized by simultaneously producing hierarchical surface structures, e.g., DLIP structure, high spatial frequency LIPSS (HSFL), and low spatial frequency LIPSS (LSFL). Also, the aspect ratio control capability of USP-DLIP is higher than that of a single Gaussian beam. Furthermore, after 4H-SiC was irradiated with USP-DLIP, the Raman results found that the peak of crystalline SiC decreased more than single-beam irradiation.

Electromagnetic origin of femtosecond laser-induced periodic surface structures on GaP crystals.

The formations of different types of laser-induced periodic surface structures (LIPSS) on the surface of GaP crystals with different laser fluence are researched in experiments. The transition from the high spatial frequency LIPSS (HSFL) to the low spatial frequency LIPSS (LSFL) occurred as the number of the irradiated laser pulse increased. The finite difference time domain method combined with the holographic ablation model is used to simulate the LIPSS formation under the irradiation of multiple pulses. Different types of ripples are predicted by the electromagnetic approach. Results demonstrate that the electromagnetic origins of HSFL and LSFL are due to the interference of incident field and the scattering field under the multi-pulse irradiation.

LIPSS Applied to Wide Bandgap Semiconductors and Dielectrics: Assessment and Future Perspectives.

With the aim of presenting the processes governing the Laser-Induced Periodic Surface Structures (LIPSS), its main theoretical models have been reported. More emphasis is given to those suitable for clarifying the experimental structures observed on the surface of wide bandgap semiconductors (WBS) and dielectric materials. The role played by radiation surface electromagnetic waves as well as Surface Plasmon Polaritons in determining both Low and High Spatial Frequency LIPSS is briefly discussed, together with some experimental evidence. Non-conventional techniques for LIPSS formation are concisely introduced to point out the high technical possibility of enhancing the homogeneity of surface structures as well as tuning the electronic properties driven by point defects induced in WBS. Among these, double- or multiple-fs-pulse irradiations are shown to be suitable for providing further insight into the LIPSS process together with fine control on the formed surface structures. Modifications occurring by LIPSS on surfaces of WBS and dielectrics display high potentialities for their cross-cutting technological features and wide applications in which the main surface and electronic properties can be engineered. By these assessments, the employment of such nanostructured materials in innovative devices could be envisaged.