Ripple formation in various metals and super-hard tetrahedral amorphous carbon films in consequence of femtosecond laser irradiation

Ripple formation in consequence of ultrashort laser pulse irradiation of materials is a well-known phenomenon. We have investigated the formation of ripples in various metals, i.e. steel, tungsten carbide hard metal, as well as in superhard ta-C films, where we used femtosecond laser pulses of 775 nm and 387 nm mean wavelength and 150 fs pulse duration. The aim was to investigate how the ripple parameters depend on irradiation parameters, and if such ripples have a potentiality for applications. In the paper, we will show that on smooth surfaces the ripple orientation is perpendicular to the electric field vector of the linearly polarized laser beam, as is well-known. Moreover, it will be shown that the ripple period decreases with decreasing laser wavelength and/or increasing angle of incidence of the laser beam on the substrate. By using optimum parameters large areas of the materials and films can be rippled swiftly, which would be important for applications. For instance, the improvement of frictional and wear behavior of tribologically stressed surfaces by ripples was investigated on ta-C coated steel surfaces.     

Progressive formation of fine and coarse ripples on SiC surface by repeated irradiation of femtosecond laser pulses

In this work, we report the progressive formation of first nanoparticles, next fine ripples, and eventually coarse ripples during the irradiation of single-crystal 6H-SiC surfaces with increasing number of femtosecond laser pulses (λ = 515 nm, τ = 250 fs, repetition rate = 100 kHz). At laser fluences greater than the single-pulse ablation threshold, nanoparticles were produced on the surface by the first few pulses over which fine ripple patterns overlapped at increased pulse numbers. As the pulse number was further increased over ten, the surface was gradually transformed into a coarse ripple–covered one. At laser fluence below the threshold, however, only fine ripples were formed nonuniformly.     

Formation of nano-textured conical microstructures in titanium metal surface by femtosecond laser irradiation

We report for the first time that a regular array of sharp nano-textured conical microstructures are formed on the titanium metal surface by irradiation with ultrafast laser pulses of 130 fs duration, 800 nm wavelength in vacuum (∼1 mbar) or in 100 mbar He. The microstructures are up to 25 μm tall, and taper to about 500 nm diameters at the tip. Irradiation in the presence of SF₆, air or HCl creates a textured surface but does not create sharp conical microstructures. The surfaces of these microstructures exhibit periodic nano-texture of feature size comparable to the wavelength of light consistent with ripple formation. Contrary to pillar formation by femtosecond laser irradiation of silicon where the initial ripples evolve into the pillars and the ripples disappear, the ripples on titanium pillars have a much smaller periodicity than the pillars and remain on the surface of the pillars. The textured surface is pitch black compared to its original silver-grayish color, i.e, it exhibits greatly reduced reflectivity throughout the measured visible spectrum. PACS 52.38.Mf; 79.20.Ds; 81.07.-b; 81.16.-c; 82.53.-k     

Pyramid-like spikes in a single crystal superalloy produced by picosecond laser irradiation

Pyramid-like spikes in a single crystal superalloy were investigated upon irradiation with picosecond (ps) laser pulses (200 ps, 800 nm, 1 kHz) under different laser fluences and pulse numbers. Both sides and grooves of pyramid-like spikes were covered with ripples, which had a period of ～760 nm. The pyramid-like spike separation increased obviously with increasing laser fluence. Microstructural investigations indicate that the pyramid-like spikes were initiated with subsequent pulses from a smooth surface with corrugations and ripples. The coexistence of capillary waves for spikes and capillary waves for ripples in the melted material can be used to explain the formation of the pyramid-like spikes.     

On the physics of self-organized nanostructure formation upon femtosecond laser ablation

We present new results on femtosecond LIPSS on silicon, fostering the dynamic model of self-organized structure formation. The first set of experiments demonstrates LIPSS formation by irradiation with a femtosecond white light continuum. The ripples are, as usual, perpendicular to the light polarization with a fluence-dependent wavelength between 500 and 700 nm. At higher dose (fluence × number of shots), the LIPSS turn to much coarser structures. The second set of experiments displays the dose dependence of pattern evolution at about threshold fluence. In contrast to the general case of multi-pulse LIPSS, where a strong dependence of the structures on the laser polarization is observed, single-shot exposition of silicon at about the ablation threshold results in a concentric pattern of very regular sub-wavelength ripples following the oval shape of the irradiated spot, without any reference to the laser polarization. When increasing the number of pulses, the usual, typical ripples develop and then coalesce into broader perpendicular structures, interlaced with remnants of the first, finer ripples.     

The growth of nanoscale periodic and dot-like structures on the surface of stainless steel with femtosecond laser pulses in the dry and wet ambient environment

The present work deals with growth of nanoscale periodic and dot-like structures on the surface of stainless steel (SS) by the irradiation of femtosecond laser pulses. For this purpose Ti: Sapphire femtosecond laser pulses (wavelength of 800 nm, pulse length of 25 fs and pulse repetition rate of 1 kHz) were employed in a dry (air) and liquid confined (deionized water and ethanol) environments. The targets were exposed to 1000 succeeding pulses for various fluences ranging from 50 to 150 mJ?cm^?2. Nanoscale structures including ripples, and dots were observed by SEM analysis. The growth and dependence of structure-formation on the ambient environment and laser fluence in both central as well as peripheral ablated areas is systematically investigated. The development of nanostructures and nanoripples is correlated with structural analysis carried out by micro Raman spectroscopy.     

Rippled area formed by surface plasmon polaritons upon femtosecond laser double-pulse irradiation of silicon: the role of carrier generation and relaxation processes

The formation of laser-induced periodic surface structures (LIPSS, ripples) upon irradiation of silicon with multiple irradiation sequences consisting of femtosecond laser pulse pairs (pulse duration 150 fs, central wavelength 800 nm) is studied numerically using a rate equation system along with a two-temperature model accounting for one- and two-photon absorption and subsequent carrier diffusion and Auger recombination processes. The temporal delay between the individual equal-energy fs-laser pulses was varied between 0 and ～4 ps for quantification of the transient carrier densities in the conduction band of the laser-excited silicon. The results of the numerical analysis reveal the importance of carrier generation and relaxation processes in fs-LIPSS formation on silicon and quantitatively explain the two time constants of the delay-dependent decrease of the low spatial frequency LIPSS (LSFL) area observed experimentally. The role of carrier generation, diffusion and recombination is quantified individually.     

Formation of a ripple pattern at a water/silicon interface using an oscillating bubble

A single femtosecond laser pulse was irradiated at a water/silicon interface, and the processed surface was investigated. Rings surrounded by ripples were found within the irradiated spot. The diameter of the rings ranged from 500 nm to 10 μm. It is proposed that acoustic waves, caused by the oscillating motion of bubbles near the water/silicon interface, deformed the melting silicon surface. In the present work, a pulse (pulse width: 150 fs) was tightly focused in water to induce optical breakdown, and a bubble was generated at an arbitrary spot. When the power density was below the ablation threshold and above the melting threshold at the silicon surface and set above the breakdown threshold at the focus in water, a pattern was generated at a specific place and with a specific size. PACS 79.20.Ds; 42.62.Cf     

时间整形飞秒激光诱导熔融硅表面纳米周期条纹的电子动力学研究

研究了时间整形飞秒激光在熔融硅表面诱导纳米周期条纹结构的电子动力学过程.通过引入非线性电离机制和表面等离子激元的瞬态作用机理,建立了关于时间整形飞秒激光诱导和调控熔融硅表面纳米周期条纹结构的电子动力学模型,并应用该模型研究获得了纳米条纹周期与时间整形脉冲时间间隔的定量关系.理论研究结果表明,通过调节时间整形脉冲的时间间隔可以实现操控表面等离子激元与激光瞬态干涉过程中的波矢配对,最终可实现对诱导的纳米条纹周期的调控.此模型预测得到的纳米条纹周期与实验结果符合得很好.该研究对于深刻理解整形脉冲链诱导材料表面纳米周期结构的电子动力学操纵机制以及对条纹周期的调控都具有重要的理论价值.     

Formation of subwavelength periodic structures on tungsten induced by ultrashort laser pulses

The evolution of surface morphology of tungsten irradiated by single-beam femtosecond laser pulses is investigated. Ripplelike periodic structures have been observed. The period of these ripples does not show a simple relation to the wavelength and angle of incidence. The orientation of ripples is aligned perpendicularly to the direction of polarization for linearly polarized light. Surprisingly, we find that the alignment of the ripple structure turned left or right by 45 degrees with respect to the incident plane when using right and left circularly polarized light, respectively. The period of the ripple can be controlled by the pulse energy, the number of pulses, and the incident angle. We find a clear threshold for the formation as a function of pulse energy and number of pulses. The mechanism for the ripple formation is discussed, as well as potential applications in large-area structuring of metals.     

Surface roughness assisted 100 kHz femtosecond laser induced nanostructure formation on silicon surface

Spontaneous nanostructure formations on roughened and smooth silicon surface by the femtosecond laser irradiation with the repetition rate of 100 kHz were systematically studied. In addition to the widely accepted so-called coarse ripple, which has the period analogous to the wavelength of the laser beam and aligns perpendicularly to the electric field of the incident laser beam, the ripple which has the period similar to the wavelength of the incident laser beam but aligns parallel to the electric field of the laser beam was observed on the roughened surface for the lower fluence and the higher number of pulse irradiation. Furthermore, the ensemble of dots formed by the enhancement of the local electric field was found on the roughened surface. This structure is preferentially formed around the scratches aligned perpendicularly to the electric field of the laser beam. These novel nanostructures are considered to be peculiar to the femtosecond laser irradiation and open the possibilities for precise control of the spontaneous nanostructure formation by femtosecond laser irradiation.     

Raman spectroscopic study of femtosecond laser-induced phase transformation associated with ripple formation on single-crystal SiC

Raman spectroscopy was performed to investigate microscopic structural changes associated with a ripple structure formation initiated by femtosecond laser irradiation on the surface of single-crystal silicon carbide. The amorphous phases of silicon carbide, silicon, and carbon were observed. The intensity ratio between amorphous silicon carbide and silicon changed discretely at the boundary between fine and coarse ripples. The physical processes responsible for the formation of the ripple structure are discussed.     

Simulation of rippled structure adjustments based on localized transient electron dynamics control by femtosecond laser pulse trains

This study investigates the effects of pulse energy distributions on subwavelength ripple structures (the ablation shapes and subwavelength ripples) using the plasma model with the consideration of laser particle–wave duality. In the case studies, the laser pulse (800 nm, 50 fs) trains consist of double pulses within a train with the energy ratios of 1:2, 1:1, and 2:1. Localized transient electron densities, material optical properties, and surface plasmon generation are strongly affected by the energy distributions. Hence, the adjustment of the ablation shape and subwavelength ripples can be achieved based on localized transient electron dynamics control during femtosecond laser pulse train processing of dielectrics. The simulation results show that better, more uniform structures, in terms of ablation shapes and subwavelength ripples, can be easily formed at a lower fluence or subpulse energy ratio of 1:1 with a fixed fluence. It is also found that pulse trains at a 1:1 energy ratio are preferred for drilling high-aspect-ratio microholes or microchannels.     

飞秒激光烧蚀硅材料表面形成周期波纹形貌研究

基于Sipe-Drude模型和表面等离子体激元(SPP)的干涉理论分别对单脉冲飞秒激光诱导硅表面形成低频率周期性波纹进行分析研究.探究了波长800 nm、脉宽150 fs的单个飞秒激光烧蚀硅造成不同激发水平下波纹形貌的变化,考虑到材料的光学性质变化(由Drude模型得到的介电常数变化),引入包含双温方程的电子数密度模型.计算结果表明,Sipe-Drude和SPP理论都适用于分析和解释高激发态下周期性波纹,但Sipe-Drude理论更适合分析更为广泛的周期性波纹结构.同时,波纹延伸方向总是垂直于入射激光偏振方向,其空间周期略小于激光波长,并受到入射激光通量的影响.在激光通量为0.38 J/cm~2时,波纹周期达到最小值.另外,还得到了不同入射角度的波纹周期变化情况,并在不同偏振态下随入射角度增大时波纹周期呈现相反的变化趋势.该研究对于理解飞秒激光造成硅表面形成周期结构及其在加工硅材料领域具有重要参考意义.     

The influence of ultra-fast temporal energy regulation on the morphology of Si surfaces through femtosecond double pulse laser irradiation

The effect of ultra-short laser-induced morphological changes upon irradiation of silicon with double pulse sequences is investigated under conditions that lead to mass removal. The temporal delay between 12 double and equal-energy pulses (E _p=0.24 J/cm² each, with pulse duration t _p=430 fs, 800 nm laser wavelength) was varied between 0 and 14 ps and a decrease of the damaged area, crater depth size and periodicity of the induced subwavelength ripples (by 3–4 %) was observed with increasing pulse delay. The proposed underlying mechanism is based on the combination of carrier excitation and energy thermalization and capillary wave solidification and aims to provide an alternative explanation of the control of ripple periodicity by temporal pulse tailoring. This work demonstrates the potential of pulse shaping technology to improve ultra-fast laser-assisted micro/nanoprocessing.     

Self-organized nanostructure by a femtosecond laser on silicon

In this paper, ripple structure and hole arrays were investigated. Techniques based on laser scanning microscopes for the processing of periodic structures on silicon with a femtosecond laser (800 nm, 1 kHz, 130 fs) had been used. Ripples and any holes were obtained after laser irradiation in air with S and P polarization. The effect of the scanning speed (v) and the lens with different numerical apertures (NA) on the laser-induced surface topography were studied. We found that the femtosecond laser produces periodic ripples on the silicon surface of the submicron level, the width of line has a tight relationship to the NA and scanning speed. Finally, we process the microapparatus on silicon, for which the wide channel was 800 nm.     

Femtosecond laser induced nanostructure formation: self-organization control parameters

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.     

Ultrafast time-resolved imaging of femtosecond laser-induced periodic surface structures on GaAs

We report the formation dynamics of periodic ripples on Ga As induced by femtosecond laser pulses（800 nm, 50 fs） via a collinear time-resolved imaging technique with a temporal resolution of 1 ps and a spatial resolution of 440 nm. The onset of periodic ripples emerges in the initial tens of picoseconds in the timescale of material ejection. The periodic ripples appear after irradiation of at least two pump pulses at surface defects produced by the first pulse and the ripple positions kept stable until the formation processes complete. The formation mechanisms of laser-induced periodic ripples are also discussed.     

不同气氛下飞秒激光诱导硅表面微结构

利用钛宝石飞秒激光脉冲对单晶硅在SF6、空气和真空环境中进行了累积脉冲辐照,研究了硅表面微结构的演化。在SF6气氛中,在激光辐照的初始阶段,硅表面形成了1维的波纹结构,随着辐照脉冲数的增加,波纹结构演化成了2维凹凸结构。累积600个脉冲后,硅表面产生了准规则排列且具有大纵横比的锥形尖峰结构。该结构呈现高度相对较低、锥形尖端小球不明显的特征,分析认为主要与环境气压的大小有关。对比空气、SF6和真空中的微结构发现,尖峰的数密度依次减小;SF6中形成的尖峰高度最大,其次为真空,再次为空气。研究结果表明,真空、SF6和空气3种环境下微结构的形成及表面形貌主要由激光烧蚀、化学刻蚀和氧化决定。     

多脉冲飞秒激光对锗材料的烧蚀效应

 开展了脉宽为40 fs的不同数量激光脉冲对锗材料的烧蚀效应实验,采用扫描电镜、激光共聚焦显微镜等方法对不同数量的飞秒激光脉冲作用下锗材料表面烧蚀区进行了检测,并对作用后材料烧蚀形貌演化规律进行了分析,初步分析了锗材料烧蚀区周围形成的不同环区的形貌特征及成因,对各环区烧蚀形貌特征随激光作用脉冲数的增加而产生的形貌演化过程进行了观测。并给出单脉冲飞秒激光对锗材料的烧蚀阈值为1.2 J·cm^-2,采用激光共聚焦显微镜测得该阈值条件下单个飞秒激光脉冲对锗材料的烧蚀深度约为150 nm。