Formation Of Laser-induced Periodic Surface Structures Research Articles

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.

Laser-driven self-organized evolution of 1D- and 2D-Nanostructures from metal thin-films on silicon: Influence of alloying and oxidation

One- and two-dimensional laser-induced periodic surface structure (LIPSS) formation of various metal (Ag, Cu, Fe, Zn, Ti) thin films on silicon wafers is achieved by irradiation with circularly polarized 532 nm nanosecond laser pulses. The occurrence and the evolution of pseudo-1D linear periodic, 2D honeycomb-like structures, and 2D periodic nanoparticle arrays were mapped for each element in dependence on the energy applied, i.e. the effective pulse number, and the metal thin film thickness. Samples series with increasing pulse counts monitor, like snapshots, the progressive pattern evolution. Because the metal thin films are of nanometer thickness only, the co-structuring of the silicon substrate must be taken into account in all cases. Even more complex are LIPSS formations on samples carrying two stacked thin films. The LIPSS formation process of thin films becomes rather complex as soon as co-structuring of the substrate, oxidation of the material, and alloy formation with substrate material or a potential second thin film layer are considered. All these effects affect the morphology of the formed LIPSS patterns.

Pulse-to-pulse ultrafast dynamics of highly photoexcited Ge2Sb2Te5 thin films

Observing ultrafast pulse-to-pulse dynamics of highly photoexcited materials could foster a comprehensive understanding of the initial stage of irreversible photoinduced events, such as phase change, structural deformation, and laser ablation. In this study, using high-repetition-rate single-shot spectroscopy and a laser microscope, the pulse-to-pulse ultrafast dynamics of energy relaxation in Ge2Sb2Te5 thin films are revealed under high-density photoexcitation that induces sequential events involving the crystalline-to-amorphous phase transition, melt and quench processes, and formation of laser-induced periodic surface structures (LIPSSs). Above the threshold excitation density for LIPSS formation, the first excitation pulse induces the transient transmittance change of the crystalline phase in a picosecond timescale, and subsequent pulses provoke the amorphous phase energy relaxation with a long decay time of hundreds of picoseconds. We observed that the subsequent pulses gradually reduce the amplitude and decay time of the transient transmittance, leading to efficient energy relaxation and LIPSS formation in the photoinduced amorphous phase.

Femtosecond Bessel beam induced ladder-like LIPSS on trimetallic surface for SERS-based sensing of Tetryl and PETN

Laser-induced periodic surface structures (LIPSS) have emerged as a potential branch of nanophotonics, offering unparalleled applications in numerous other research fields such as on-chip microelectronics, hydrogen evolution, solar-energy conversion, photodetectors, photocatalysis, and sensing. In this study, for the first time, we have created novel, Ag-Au-Cu alloyed trimetallic, ladder-like LIPSS nanostructures engaging an axicon-generated femtosecond Bessel beam. The LIPSS formation mechanism through modulation of ablation fluence profile, involving interference of photon-induced surface plasmon polariton with incident beam, has been meticulously divulged. The overlapping feature of Bessel beam profiles has been considered to improve the coupling of electromagnetic modes with the pre-patterned surfaces. The period (Λ) of the fabricated low spatial frequency LIPSS has been estimated to be 540 ± 12 nm. Also, as a comparative study, the distinct topographical features of nanostructures generated under a Gaussian beam with an identical fluence has also been presented. Additionally, these trimetallic plasmonic nanostructures have demonstrated outstanding excellence as active surface-enhanced Raman scattering substrates for sensing applications. Traces (200 nM) of real-time explosives such as Tetryl and pentaerythritol tetranitrate (PETN) have been detected, while achieving enhancement factors in the range of 105, making these viable for practical applications.

Femtosecond laser structuring in the fabrication of periodic nanostructure on titanium for enhanced photoelectrochemical dopamine sensing performance

Femtosecond laser structuring in the fabrication of periodic nanostructure on titanium for enhanced photoelectrochemical dopamine sensing performance was reported. The formation of laser induced periodic surface structures (LIPSS) upon titanium foil depended on the polarization of the femtosecond laser beam. When linearly and radially polarized femtosecond laser beam interacted with titanium foil, LIPSS were generated on titanium surface and further used for the fabrication of electrode material in photoelectrochemical dopamine sensing. Field emission scanning electron microscopy (FESEM), X-ray photoelectron spectroscopy (XPS), and UV–vis absorption spectra were performed to study the surface characteristics of the laser treated titanium foil. The results revealed that low spatial frequency LIPSS (LSFL) formation occurred at both cases of the linearly and radially polarized laser treated titanium foil with a period of about 350 and 250 nm and owned the significant surface chemical and structural modification (abundant Ti4+ state and hydroxyl functional group), especially in term of radially polarized laser treated titanium foil. The radially polarized laser treated titanium foil owning optimal surface structural modification contributed multiple catalytically active sites and made the outstanding photoelectrochemical performance of dopamine sensing. It was concluded that femtosecond laser surface structuring made it possible to modify the surface characteristics of objects for future construction of sensing platforms.

Femtosecond Laser-Induced Periodic Surface Structures in Titanium-Doped Diamond-like Nanocomposite Films: Effects of the Beam Polarization Rotation.

We study the properties of laser-induced periodic surface structures (LIPSS) formed on titanium-doped diamond-like nanocomposite (DLN) a-C:H:Si:O films during ablation processing with linearly-polarized beams of a visible femtosecond laser (wavelength 515 nm, pulse duration 320 fs, pulse repetition rates 100 kHz-2 MHz, scanning beam velocity 0.05-1 m/s). The studies are focused on (i) laser ablation characteristics of Ti-DLN films at different pulse frequencies and constant fluence close to the ablation threshold, (ii) effects of the polarization angle rotation on the properties of low spatial frequency LIPSS (LSFL), and (iii) nanofriction properties of the 'rotating' LIPSS using atomic force microscopy (AFM) in a lateral force mode. It is found that (i) all LSFL are oriented perpendicular to the beam polarization direction, so being rotated with the beam polarization, and (ii) LSFL periods are gradually changed from 360 ± 5 nm for ripples parallel to the beam scanning direction to 420 ± 10 nm for ripples formed perpendicular to the beam scanning. The obtained results are discussed in the frame of the surface plasmon polaritons model of the LIPSS formation. Also, the findings of the nanoscale friction behavior, dependent on the LIPSS orientation relative to the AFM tip scanning direction, are presented and discussed.

Influence of film thickness and substrate roughness on the formation of laser induced periodic surface structures in poly(ethylene terephthalate) films deposited over gold substrates

A study of the formation of Laser Induced Periodic Surface Structures (LIPSS) using near-infrared femtosecond pulsed laser irradiation on poly(ethylene terephthalate) (PET) films deposited over gold substrates has been carried out. We report the influence of the gold substrate roughness and the PET film thickness on LIPSS formation and analyze it in terms of the features of the electric field distribution obtained by computer simulations using COMSOLTM. We obtain LIPSS with periods close to the irradiation wavelength as long as the aforementioned substrate and film parameters remain below certain threshold values, in particular for polymer thicknesses below 200 nm and substrate roughness of few nm. However, experiments show the impossibility of LIPSS formation for rough substrates as well as thick films above these threshold values. In our numerical simulations, we notice the generation of Surface Plasmon Polariton (SPP) in the film-substrate interface that gives rise to a periodical field pattern on the surface of the thin film. This periodicity is broken for a certain level of substrate roughness or film thickness. Moreover, the evolution of the period of the SPP as the substrate roughness and film thickness change for given laser parameters is qualitatively in good agreement with the experimental LIPSS period (below but close to the irradiation laser wavelength). In conclusion, the experimental findings are explained by the formation and behavior of SPP in the thin film-substrate interface. On these grounds, we propose that, for our case of study, this SPP formation and the subsequent inhomogeneous rise in temperature induced by the periodic field on the surface of the sample is the leading mechanism contributing to LIPSS formation.

Physicochemical Modifications on Thin Films of Poly(Ethylene Terephthalate) and Its Nanocomposite with Expanded Graphite Nanostructured by Ultraviolet and Infrared Femtosecond Laser Irradiation

In this work, the formation of laser-induced periodic surface structures (LIPSS) on the surfaces of thin films of poly(ethylene terephthalate) (PET) and PET reinforced with expanded graphite (EG) was studied. Laser irradiation was carried out by ultraviolet (265 nm) and near-infrared (795 nm) femtosecond laser pulses, and LIPSS were formed in both materials. In all cases, LIPSS had a period close to the irradiation wavelength and were formed parallel to the polarization of the laser beam, although, in the case of UV irradiation, differences in the formation range were observed due to the different thermal properties of the neat polymer in comparison to the composite. To monitor the modification of the physicochemical properties of the surfaces after irradiation as a function of the laser wavelength and of the presence of the filler, different techniques were used. Contact angle measurements were carried out using different reference liquids to measure the wettability and the solid surface free energies. The initially hydrophilic surfaces became more hydrophilic after ultraviolet irradiation, while they evolved to become hydrophobic under near-infrared laser irradiation. The values of the surface free energy components showed changes after nanostructuring, mainly in the polar component. Additionally, for UV-irradiated surfaces, adhesion, determined by the colloidal probe technique, increased, while, for NIR irradiation, adhesion decreased. Finally, nanomechanical properties were measured by the PeakForce Quantitative Nanomechanical Mapping method, obtaining maps of elastic modulus, adhesion, and deformation. The results showed an increase in the elastic modulus in the PET/EG, confirming the reinforcing action of the EG in the polymer matrix. Additionally, an increase in the elastic modulus was observed after LIPSS formation.

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

Laser-induced periodic surface structures formation and reversible crystallization in amorphous Ge2Sb2Te5 thin films as a result of femtosecond irradiation

Laser-induced periodic surface structures formation and reversible crystallization in amorphous Ge2Sb2Te5 thin films as a result of femtosecond irradiation

Femtosecond large-area fabrication of multi-phase titanium oxide LIPSS on thin films

The effect of the laser beam scanning velocity and overlap on the large-area fabrication of Laser-Induced Periodic Surface Structures (LIPSS), on 400 nm thickness titanium films, is investigated. The experiments were performed in ambient air with well below ablation threshold laser fluence by using a femtosecond laser at a wavelength of 1030 nm with a pulse duration of 270 fs, operating at a repetition rate of 20 kHz.For this purpose, single-line experiments were performed to study the LIPSS formation process as a function of fs-laser-beam scanning velocity. Based on these results, the fabrication of large-area LIPSS pattern was investigated by unidirectional scanning of the fs-laser beam across the sample surface using different lateral spacing. The results show the formation of LSFL and TLIPSS, with different orientation with respect to the polarization of the incident radiation. The analysis of the chemical composition, by microRaman spectroscopy, indicates the formation of a mixture of TiO2 (anatase phase) and Ti2O3 (rutile phase) for high scanning velocities and TiO2 (rutile phase) for low scanning velocities. The chemical composition, spatial period, and depth of the LIPSS show a clear dependence with the laser-beam scanning velocity and overlap.

Controlling LIPSS formation on Ni surface using near-infrared laser beam and its low-order harmonics

Ultrafast laser ablation of metal surfaces is a common physical process used to generate periodic surface structures with tuneable multifunctionality for various applications in science and technology. In this work, the formation of femtosecond laser-induced periodic surface structures (LIPSSs) is investigated with 50 kHz repetition rate laser of 40 fs pulse duration and a central wavelength () along with its second () and third ) harmonic components. The variation in the LIPSS periodicity is demonstrated by changing the wavelength of the ablating laser pulses. LIPSS with periodicity ∼0.85 m at the fundamental ablating pulses, ∼0.42 m periodicity at the second harmonic, and ∼0.35 m periodicity at the third harmonic were observed. The third harmonic radiation was generated in an air-filament with minimal temporal delay with respect to the fundamental driving pulses to structure Nickel surfaces at ambient conditions. The approach demonstrates the potential for generating very fine LIPSS on materials’ surfaces using the efficient high-order harmonics of an infrared fundamental laser beam.

Self-induced decay of intense laser pulse into a pair of surface plasmons

We show theoretically that an intense femtosecond optical pulse incident normally on a metal surface tends to decay into a pair of counterpropagating surface plasmon polaritons (SPPs). The interference field heats the medium periodically, which causes a periodic permittivity perturbation and, in turn, resonantly amplifies the magnitudes of the SPPs. The instability growth time is 10--50 fs for typical metals at laser fluences of about $\ensuremath{\sim}1\phantom{\rule{0.16em}{0ex}}\mathrm{J}/{\mathrm{cm}}^{2}$, so this mechanism is important for understanding the dynamics of the optical pulse absorption under damaging conditions, and it is promising for the interpretation of laser-induced periodic surface structure formation in single- and few-pulse pumping regimes.

Synergy of electromagnetic effects and thermophysical properties of metals in the formation of laser-induced periodic surface structures

Femtosecond (fs) pulsed lasers have been widely used over the past few decades for precise materials structuring at the micro- and nano-scales. However, in order to realize efficient material processing and account for the formation of laser-induced periodic surface structures (LIPSS), it is very important to understand the fundamental laser–matter interaction processes. A significant contribution to the LIPSS profile appears to originate from the electromagnetic fingerprint of the laser source. In this work, we follow a systematic approach to predict the pulse-by-pulse formation of LIPSS on metals due to the development of a spatially periodic energy deposition that results from the interference of electromagnetic far fields on a non-flat surface profile. On the other hand, we demonstrate that the induced electromagnetic effects alone are not sufficient to allow the formation of LIPSS, therefore we emphasize the crucial role of electron diffusion and electron–phonon coupling on the formation of stable periodic structures. Gold (Au) and stainless steel (SS) are considered as two materials to test the theoretical model while simulation results appear to confirm the experimental results that, unlike with Au, fabrication of pronounced LIPSS on SS is feasible.

Research on Monocrystalline Silicon Micro-Nano Structures Irradiated by Femtosecond Laser.

Femtosecond (fs) laser processing has received great attention for preparing novel micro-nano structures and functional materials. However, the induction mechanism of the micro-nano structures induced by fs lasers still needs to be explored. In this work, the laser-induced periodic surface structure (LIPSS) of monocrystalline silicon (Si) under fs laser irradiation is investigated. Three different layers named amorphous silicon (a-Si) layer, transition layer, and unaffected Si layer are observed after laser irradiation. The a-Si layer on the surface is generated by the resolidification of melting materials. The unaffected Si layer is not affected by laser irradiation and maintains the initial atomic structure. The transition layer consisting of a-Si and unaffected Si layers was observed under the irradiated subsurface. The phase transition mechanism of Si irradiated by fs laser is “amorphous transition”, with the absence of other crystal structures. A numerical model is established to describe the fs laser-Si interaction to characterize the electronic (lattice) dynamics of the LIPSS formation. The obtained results contribute to the understanding of fs laser processing of Si at the atomic scale as well as broaden the application prospects of fs laser for treating other semiconductor materials.

Uniformity Control of Laser-Induced Periodic Surface Structures

Laser-induced periodic surface structures (LIPSSs) are a universal phenomenon that can be observed on a variety of materials, including metals, semiconductors, and dielectrics, upon irradiation with ultrafast laser pulses. It has found various potential applications in the fields of optics, biologics, and mechatronics due to its efficient and flexible fabrication process and subwavelength quasi-periodic property. However, LIPSSs face the challenge of uniformity control because the formation of micro-/nanostructures induced by ultrafast laser is a complex process involving multiple interacting factors, including laser energy deposition, phase change, light scattering, and instantaneous local changes of material properties and their feedback mechanisms. Recently, there has been some significant progress regarding the control of LIPSS uniformity. In this work, we review recent experimental and methodological advances on this topic from three aspects: 1) laser-induced modified-LIPSS, 2) feedback mechanism of LIPSS formation, and 3) ultrafast laser pulse shaping. This review can stimulate further investigations into the uniformity control of LIPSSs to support and accelerate the industrial applications of uniform LIPSSs.

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”.

The influence of processing environment on laser-induced periodic surface structures generated with green nanosecond laser

Laser-induced periodic surface structures (LIPSS) are nanometric surface undulations produced by short and ultrashort pulsed lasers. The production of high-quality LIPSS is essential to obtain the required surface responses in various applications. In this work, the LIPSS were fabricated on stainless steel surfaces by a 515 nm nanosecond laser operating under ambient and argon enriched atmospheres to investigate their quality. The LIPSS quality is correlated to the diffracted light intensity and their key geometric parameters such as periodicity and amplitude. The LIPSS formation was observed at an accumulated fluence of above 13.9 J/cm2 and the optimal processing window was sustained up to 46.2 J/cm2 before the oxidation occurred. The LIPSS generated in the argon environment exhibited a relatively higher intensity of the diffracted light than those processed in the ambient conditions. Furthermore, LIPSS generated in argon showed minimum surface defects and higher amplitude ripples compared to those in air. The X-ray photoelectron spectroscopy analysis revealed that the ratio of oxygen to metal species decreased in the argon atmosphere and thus minimal surface oxidation occurred on the samples. Since the generation of high-quality LIPSS is a prerequisite for an accurate predictive modeling of surface responses, the results reported here show that good nanostructured surfaces can be produced with cost-effective nanosecond green lasers.

Generation of micro/nano hybrid surface structures on copper by femtosecond pulsed laser irradiation

The delamination of copper lead frames from epoxy molding compounds (EMC) is a severe problem for microelectronic devices, as it leads to reduced heat dissipation or circuit breakage. The micro/nanoscale surface structuring of copper is a promising method to improve the copper–EMC interfacial adhesion. In this study, the generation of micro/nano hybrid structures on copper surfaces through femtosecond pulsed laser irradiation is proposed to improve interfacial adhesion. The micro/nano hybrid structures were realized by generating nanoscale laser-induced periodic surface structures (LIPSS) on microscale parallel grooves. Several types of hybrid surface structures were generated by changing the laser polarization direction, fluence, and scanning speed. At a specific aspect ratio of microgrooves, a latticed structure was generated on the sides of microgrooves by combining LIPSS formation and direct laser interference patterning. This study provides an efficient method for the micro/nanoscale hybrid surface structure formation for interfacial adhesion improvement between copper and EMC.

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.