Ultrafast dynamics of femtosecond laser-induced high spatial frequency periodic structures on silicon surfaces

Femtosecond laser-induced periodic surface structures(LIPSS)have been extensively studied over the past few decades.In particular,the period and groove width of high-spatial-frequency LIPSS(HSFL)is much smaller than the diffraction limit,making it a useful method for efficient nanomanufacturing.However,compared with the low-spatial-frequency LIPSS(LSFL),the structure size of the HSFL is smaller,and it is more easily submerged.Therefore,the formation mechanism of HSFL is complex and has always been a research hotspot in this field.In this study,regular LSFL with a period of 760 nm was fabricated in advance on a silicon surface with two-beam interference using an 800 nm,50 fs femtosecond laser.The ultrafast dynamics of HSFL formation on the silicon surface of prefabricated LSFL under single femtosecond laser pulse irradiation were observed and analyzed for the first time using collinear pump-probe imaging method.In general,the evolution of the surface structure undergoes five sequential stages:the LSFL begins to split,becomes uniform HSFL,degenerates into an irregular LSFL,undergoes secondary splitting into a weakly uniform HSFL,and evolves into an irregular LSFL or is submerged.The results indicate that the local enhancement of the submerged nanocavity,or the nanoplasma,in the prefabricated LSFL ridge led to the splitting of the LSFL,and the thermodynamic effect drove the homogenization of the splitting LSFL,which evolved into HSFL.

Two-dimensional laser-induced periodic surface structures formed on crystalline silicon by GHz burst mode femtosecond laser pulses

Femtosecond laser pulses with GHz burst mode that consist of a series of trains of ultrashort laser pulses with a pulse interval of several hundred picoseconds offer distinct features in material processing that cannot be obtained by the conventional irradiation scheme of femtosecond laser pulses(single-pulse mode).However,most studies using the GHz burst mode femtosecond laser pulses focus on ablation of materials to achieve high-efficiency and high-quality material removal.In this study,we explore the ability of the GHz burst mode femtosecond laser processing to form laser-induced periodic surface structures(LIPSS)on silicon.It is well known that the direction of LIPSS formed by the single-pulse mode with linearly polarized laser pulses is typically perpendicular to the laser polarization direction.In contrast,we find that the GHz burst mode femtosecond laser(wavelength:1030 nm,intra-pulse duration:220 fs,intra-pulse interval time(intra-pulse repetition rate):205 ps(4.88 GHz),burst pulse repetition rate:200 kHz)creates unique two-dimensional(2D)LIPSS.We regard the formation mechanism of 2D LIPSS as the synergetic contribution of the electromagnetic mechanism and the hydrodynamic mechanism.Specifically,generation of hot spots with highly enhanced electric fields by the localized surface plasmon resonance of subsequent pulses in the bursts within the nanogrooves of one-dimensional LIPSS formed by the preceding pulses creates 2D LIPSS.Additionally,hydrodynamic instability including convection flow determines the final structure of 2D LIPSS.

Large-area straight,regular periodic surface structures produced on fused silica by the interference of two femtosecond laser beams through cylindrical lens

Inhomogeneity and low efficiency are two important factors that limit the application of laser-induced periodic surface structures(LIPSSs),especially on glass surfaces.In this study,two-beam interference(TBI)of femtosecond lasers was used to produce large-area straight LIPSSs on fused silica using cylindrical lenses.Compared with those produced us-ing a single circular or cylindrical lens,the LIPSSs produced by TBI are much straighter and more regular.Depending on the laser fluence and scanning velocity,LIPSSs with grating-like or spaced LIPSSs are produced on the fused silica sur-face.Their structural colors are blue,green,and red,and only green and red,respectively.Grating-like LIPSS patterns oriented in different directions are obtained and exhibit bright and vivid colors,indicating potential applications in surface coloring and anti-counterfeiting logos.

Enhancement of photocatalytic activity by femtosecond-laser induced periodic surface structures of Si

Laser induced periodic surface structures(LIPSS)represent a kind of top down approach to produce highly reproducible nano/microstructures without going for any sophisticated process of lithography.This method is much simpler and cost effective.In this work,LIPSS on Si surfaces were generated using femtosecond laser pulses of 800 nm wavelength.Photocatalytic substrates were prepared by depositing TiO2 thin films on top of the structured and unstructured Si wafer.The coatings were produced by sputtering from a Ti target in two different types of oxygen atmospheres.In first case,the oxygen pressure within the sputtering chamber was chosen to be high(3×10^–2 mbar)whereas it was one order of magnitude lower in second case(2.1×10^–3 mbar).In photocatalytic dye decomposition study of Methylene blue dye it was found that in the presence of LIPSS the activity can be enhanced by 2.1 and 3.3 times with high pressure and low pressure grown TiO2 thin films,respectively.The increase in photocatalytic activity is attributed to the enlargement of effective surface area.In comparative study,the dye decomposition rates of TiO2 thin films grown on LIPSS are found to be much higher than the value for standard reference thin film material Pilkington Activ^TM.

Laser-induced periodic surface structured electrodes with 45% energy saving in electrochemical fuel generation through field localization

Electrochemical oxidation/reduction of radicals is a green and environmentally friendly approach to generating fuels.These reactions,however,suffer from sluggish kinetics due to a low local concentration of radicals around the electrocatalyst.A large applied electrode potential can enhance the fuel generation efficiency via enhancing the radical concentration around the electrocatalyst sites,but this comes at the cost of electricity.Here,we report about a~45%saving in energy to achieve an electrochemical hydrogen generation rate of 3×10^(16) molecules cm^(–2)s^(–1)(current density:10 mA/cm^(2))through localized electric field-induced enhancement in the reagent concentration(LEFIRC)at laser-induced periodic surface structured(LIPSS)electrodes.The finite element model is used to simulate the spatial distribution of the electric field to understand the effects of LIPSS geometric parameters in field localization.When the LIPSS patterned electrodes are used as substrates to support Pt/C and RuO_(2) electrocatalysts,the η_(10) overpotentials for HER and OER are decreased by 40.4 and 25%,respectively.Moreover,the capability of the LIPSS-patterned electrodes to operate at significantly reduced energy is also demonstrated in a range of electrolytes,including alkaline,acidic,neutral,and seawater.Importantly,when two LIPSS patterned electrodes were assembled as the anode and cathode into a cell,it requires 330 mVs of lower electric potential with enhanced stability over a similar cell made of pristine electrodes to drive a current density of 10 mA/cm^(2).This work demonstrates a physical and versatile approach of electrode surface patterning to boost electrocatalytic fuel generation performance and can be applied to any metal and semiconductor catalysts for a range of electrochemical reactions.

Femtosecond laser-induced periodic surface structures on hard and brittle materials

Hard and brittle materials have high hardness,excellent optical stability,chemical stability,and high thermal stability.Hence,they have huge application potential in various fields,such as optical components,substrate materials,and quantum information,especially under harsh conditions,such as high temperatures and high pressures.Femtosecond laser direct writing technology has greatly promoted the development of femtosecond laser-induced periodic surface structure(Fs-LIPSS or LIPSS by a femtosecond laser)applications of hard and brittle materials due to its high precision,controllability,and three-dimensional processing ability.Thus far,LIPSSs have been widely used in material surface treatment,optoelectronic devices,and micromechanics.However,a consensus has not been reached regarding the formation mechanism of LIPSSs on hard and brittle materials.In this paper,three widely accepted LIPSS formation mechanisms are introduced,and the characteristics and applications of LIPSSs on diamonds,silicon,silicon carbide,and fused silica surfaces in recent years are summarized.In addition,the application prospects and challenges of LIPSSs on hard and brittle materials by a femtosecond laser are discussed.

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.

Heat accumulation effects in femtosecond laser-induced subwavelength periodic surface structures on silicon

High-repetition rate femtosecond lasers are shown to drive heat accumulation processes that are attractive for femtosecond laser-induced subwavelength periodic surface structures on silicon.Femtosecond laser micromachining is no longer a nonthermal process,as long as the repetition rate reaches up to 100 kHz due to heat accumulation.Moreover,a higher repetition rate generates much better defined ripple structures on the silicon surface,based on the fact that accumulated heat raises lattice temperature to the melting point of silicon(1687 K),with more intense surface plasmons excited simultaneously.Comparison of the surface morphology on repetition rate and on the overlapping rate confirms that repetition rate and pulse overlapping rate are two competing factors that are responsible for the period of ripple structures.Ripple period drifts longer because of a higher repetition rate due to increasing electron density;however,the period of laser structured surface is significantly reduced with the pulse overlapping rate.The Maxwell–Garnett effect is confirmed to account for the ripple period-decreasing trend with the pulse overlapping rate.

Nanosecond laser-induced controllable periodical surface structures on silicon

In this paper,an effective method is proposed to generate specific periodical surface structures.A 532 nm linearly polarized laser is used to irradiate the silicon with pulse duration of 10 ns and repetition frequency of 10 Hz.Laser-induced periodic surface structures(LIPSSs) are observed when the fluence is 121 mJ/cm;and the number of pulses is 1000.The threshold of fluence for generating LIPSS gradually increases with the decrease of the number of pulses.In addition,the laser incident angle has a notable effect on the period of LIPSS,which varies from 430 nm to 1578 nm,as the incident angle ranges from10° to 60° correspondingly.Besides,the reflectivity is reduced significantly on silicon with LIPSS.

Impact of flm thickness in laser‑induced periodic structures on amorphous Si flms

We report self-organized periodic nanostructures on amorphous silicon thin flms by femtosecond laser-induced oxidation.The dependence of structural periodicity on the thickness of silicon flms and the substrate materials is investigated.The results reveal that when silicon flm is 200 nm,the period of self-organized nanostructures is close to the laser wavelength and is insensitive to the substrates.In contrast,when the silicon flm is 50 nm,the period of nanostructures is much shorter than the laser wavelength,and is dependent on the substrates.Furthermore,we demonstrate that,for the thick silicon flms,quasi-cylindrical waves dominate the formation of periodic nanostructures,while for the thin silicon flms,the formation originates from slab waveguide modes.Finite-diference time-domain method-based numerical simulations support the experimental discoveries.

Surface Micro-Nano Structures on GaN Thin Films Induced by 355 nm Nanosecond Laser Irradiation

Gallium nitride(GaN)has widespread applications in the semiconductor industry because of its desirable optoelectronic properties.The fabrication of surface structures on GaN thin films can effectively modify their optical and electrical properties,providing additional degrees of freedom for controlling GaN-based devices.Compared with lithography-based techniques,laser processing is maskless and much more efficient.This paper shows how surface micronano structures can be produced on GaN thin films using 355 nm nanosecond laser irradiation.The effects of the laser pulse energy,number of pulses,and polarization direction were studied.It was found that distinct micro-nano structures were formed under different irradiation conditions,and their geometries and elemental compositions were analyzed.The results indicate that different types of surface micro-nano structures can be produced on GaN thin films in a controllable manner using 355 nm nanosecond laser irradiation.The results of our study provide valuable guidance for the surface modification of GaN-based optoelectronic devices.

Investigations on femtosecond laser-induced surface modification and periodic micropatterning with anti-friction properties on Ti6Al4V titanium alloy

Titanium alloys have a wide application in aerospace industries as it has greater strength and low density, but it has poor tribological properties. To improve its friction and wear performance, in present work, a femtosecond laser is used to directly irradiate the Ti6Al4V titanium alloy surface in air conditioning, which results in localized ablation and the formation of periodic microstructures but also a strong pressure wave, propagating the material inside. Through the optimization of processing parameters, surface modification and periodic micropatterning with effective anti-friction properties were successfully induced on the surface. After a treatment of femtosecond laser-induced surface modification(FsLSM), the surface microhardness was improved by 16.6% and compressive residual stress reached-746 MPa. Besides, laser-induced periodic surface structures(LIPSS) with a titanium oxide outer coating were fabricated uniformly on the titanium alloy surface. Rotary ball-on-disk wear experiments revealed that the average coefficient of friction(COF) and wear mass loss of the specimen with Fs LSM treatment were largely reduced by 68.9% and 90% as compared to that of untreated specimens, respectively. It was analyzed that the reason for the remarkable wear resistance was attributed to the comprehensive action of the generation of LIPSS, the titanium oxide outer coating, high amplitude compressive residual stress and gradient grain size distribution on the subsurface during the laser surface treatment. Since the findings here are broadly applicable to a wide spectrum of engineering metals and alloys, the present results offer unique pathways to enhancing the tribological performance of materials.

Periodic surface functional group density on graphene via laserinduced substrate patterning at Si/SiO2 interface

Controlling the spatial distribution of functional groups on two-dimensional(2D)materials on a micrometer scale and below represents a fascinating opportunity to achieve anisotropic(opto)electronic properties of these materials.Periodic patterns of covalent functionalization can lead to pericxJic potentials in the monolayer;however,creating such superstructures is very challenging.Here,we describe an original approach to the periodic functionalization of graphene induced by substrate patterning using a pulsed laser.Laser-induced periodic surface structures(LIPSS)are produced on silicon wafers with thermally-grown oxide layers.The irradiation conditions for the formation of UPSS confined at the SiO2/Si interface have been unravelled.LIPSS imprint their periodicity to the reactivity of the monolayer graphene placed on the substrate via modulation of its local doping level.This method is clean,straightforward and scalable with high spatial resolution.

Gyroid Triply Periodic Minimal Surface Lattice Structure Enables Improved Superelasticity of CuAlMn Shape Memory Alloy

Improving the shape memory effect and superelasticity of Cu-based shape memory alloys(SMAs)has always been a research hotspot in many countries.This work systematically investigates the effects of Gyroid triply periodic minimal surface(TPMS)lattice structures with different unit sizes and volume fractions on the manufacturing viability,compressive mechanical response,superelasticity and heating recovery properties of CuAlMn SMAs.The results show that the increased specific surface area of the lattice structure leads to increased powder adhesion,making the manufacturability proportional to the unit size and volume fraction.The compressive response of the CuAlMn SMAs Gyroid TPMS lattice structure is negatively correlated with the unit size and positively correlated with the volume fraction.The superelastic recovery of all CuAlMn SMAs with Gyroid TPMS lattice structures is within 5%when the cyclic cumulative strain is set to be 10%.The lattice structure shows the maximum superelasticity when the unit size is 3.00 mm and the volume fraction is 12%,and after heating recovery,the total recovery strain increases as the volume fraction increases.This study introduces a new strategy to enhance the superelastic properties and expand the applications of CuAlMn SMAs in soft robotics,medical equipment,aerospace and other fields.

High period frequency LIPSS emerging on 304 stainless steel under the irradiation of femtosecond laser double-pulse trains

In this work,we used femtosecond laser double-pulse trains to produce laser-induced periodic surface structures(LIPSS)on 304 stainless steel.Surprisingly,a novel type of periodic structure was discovered,which,to the best of our knowledge,is the first in literature.We surmised that the cause for this novel LIPSS was related to the weak energy coupling of subpulses when the intrapulse delay was longer than the thermal relaxation time of stainless steel.Furthermore,we found that the fluence combination and arrival sequence of subpulses in a double-pulse train also influenced LIPSS morphology.

Laser ablation and structuring of CdZnTe with femtosecond laser pulses

We report an experimental investigation on laser ablation and associated surface structuring of CdZnTe by femtosecond Ti:Sa laser pulses(laser wavelengthλ≈800 nm,≈35 fs,10 Hz),in air.By exploiting different static irradiation conditions,the fluence threshold and the incubation effect in CdZnTe are estimated.Interestingly,surface treatment with a low laser fluence(laser pulse energy E≈5-10_μJ)and number of shots(5<N<50)show the formation of well-defined cracks in the central part of the shallow crater,which is likely associated to a different thermal expansion coefficients of Te inclusions and matrix during the sample heating and cooling processes ensuing femtosecond laser irradiation.Irradiation with a larger number of pulses(N≈500,1000)with higher pulse energies(E≈30-50μJ)results in the formation of welldefined laser-induced periodic surface structures(LIPSS)in the outskirts of the main crater,where the local fluence is well below the material ablation threshold.Both low spatial frequency and high spatial frequency LIPSS perpendicular to the laser polarization are found together and separately depending on the irradiation condition.These are ascribed to a process of progressive aggregation of randomly distributed nanoparticles produced during laser ablation of the deep crater in the region of the target irradiated by a fluence below the ablation threshold with many laser pulses.