Analysis of plume deflection in the silicon laser ablation process

Changes in target surface morphology and ablation plume direction have been experimentally observed during the initial stages of the silicon laser ablation process. A relationship between both phenomena can be observed upon analysing the temperature field induced by the laser beam in a rough surface material. Theoretical studies on the deflection of the ablation plume are presented. These analyses are based on the hypothesis that particles that reach evaporation temperature will exit normally to the target surface with a velocity that is proportional to the surface temperature and the amount of the ablated material. Numerical solutions and experimental results of laser ablation process of silicon targets are found to agree with theoretical studies. PACS 42.25.Lc; 79.20.Dc; 02.70.Dc     

Nanosecond and femtosecond ablation of La0.6Ca0.4CoO3: a comparison between plume dynamics and composition of the films

Thin films of La_0.6Ca_0.4CoO₃ were grown by pulsed laser ablation with nanosecond and femtosecond pulses. The films deposited with femtosecond pulses (248 nm, 500 fs pulse duration) exhibit a higher surface roughness and deficiency in the cobalt content compared to the films deposited with nanosecond pulses (248 nm, 20 ns pulse duration). The origin of these pronounced differences between the films grown by ns and fs ablation has been studied in detail by time-resolved optical emission spectroscopy and imaging. The plumes generated by nanosecond and femtosecond ablation were analyzed in vacuum and in a background pressure of 60 Pa of oxygen. The ns-induced plume in vacuum exhibits a spherical shape, while for femtosecond ablation the plume is more elongated along the expansion direction, but with similar velocities for ns and fs laser ablation. In the case of ablation in the background gas similar velocities of the plume species are observed for fs and ns laser ablation. The different film compositions are therefore not related to different kinetic energies and different distributions of various species in the plasma plume which has been identified as the origin of the deficiency of species for other materials.     

Optical transmission and reflection of aluminum film irradiated by nanosecond laser beam and experimental studying of phase-explosion

In this paper we present evidence for a phase explosion during the laser-induced ablation process by studying the optical reflectivity of the ablated plume. The ablation was produced by irradiating thin film aluminum coated on a quartz substrate with a single pulse laser beam in ambient air. The laser pulse was provided by the second harmonic of a Q-switched Nd:YAG laser with ∼10 ns pulse duration. The transmission of a low power He–Ne laser beam through the hot ablated material plume and its reflection (from the front surface, and rear surface of aluminum film) were also monitored during the duration of the ablation event. The results show that the front surface reflectivity is enhanced at an early time of ablation which is described as strong evidence for the creation of a phase explosion in this process.     

Measurement of laser beam transmittance through laser produced vapour plume

Laser produced plume, consisting of vapor front and ejected substrate on the workpiece surface, is an intermediate between the incident laser beam and the workpiece on which the beam is directed. It partially blocks, defocuses, absorbs, scatters, and deflects the incident beam and thereby reduces the laser energy reaching the workpiece. However, plume additionally acts as a heat source enhancing the machining. Consequently, laser induced plume plays an important role in laser machining process. The present study investigates the transmittance of a reference beam by the plume generated during the laser-workpiece interaction. To achieve the transmittance measurements, a Nd:YAG laser was used and four different materials were employed in the experiment. To obtain realistic values of the plume transmittance in relation to the laser machining process, the reference beam was sampled from the incident laser beam. The study was extended to include the effect of the laser pulse parameters on the transmission process. It is found that about 10–30% of the transmittance of the reference beam through a vapor plume, produced due to laser ablation, occurs close to the workpiece surface.     

Phase explosion and recoil-induced ejection in resonant-infrared laser ablation of polystyrene

We investigate the phenomenon of resonant-infrared laser ablation of polymers using polystyrene as a model material. Ablation is carried out using various mid-IR laser wavelengths that are resonant with vibrational modes of a polystyrene target. Time-resolved plume imaging coupled with etch-depth measurements and thermal calculations indicate that ablation begins after a superheated surface layer reaches a temperature of ∼1000°C and undergoes spinodal decomposition. The majority of the ablated material is then expelled by way of recoil-induced ejection as the pressure of the expanding vapor plume compresses a laser-melted area.     

Effects of laser operating parameters on metals micromachining with ultrafast lasers

180 femtoseconds (1 kHz) and 10 picoseconds (1-50 kHz) ultrafast laser micro-structuring of the metals Ti alloy, Al and Cu have been studied for the purpose of industrial application. The effects of some key laser operating parameters were investigated. The evolution of surface morphology revealed that laser pulses overlap in a range around the spatial FWHM can help to achieve optimal residual surface roughness. While observed ablation rate (unit: μm³ per pulse) changed dramatically with repetition rate due to the combined effects of plasma absorption, residual thermal energy and phase transition, higher throughput can be achieved with higher repetition rate. This study also indicated that residual surface roughness is almost independent of repetition rate at 10 ps temporal pulse length. The ablation depth is approximately proportional to the number of overscan; however, machining accuracy deteriorates, especially for femtosecond laser processing and metals with low thermal conductivity and short electron-phonon coupling time.     

Carbon-plasma produced in vacuum by 532 nm-3 ns laser pulses ablation

A study of VIS laser ablation of graphite, in vacuum, by using 3 ns Nd:YAG laser radiation is reported. Nanosecond pulsed ablation gives an emission mass spectrum attributable to C_n neutral and charged particles. Mass quadrupole spectroscopy, associated to electrostatic ion deflection, allows estimation of the velocity distributions of several of these emitting species within the plume as a function of the incident laser fluence. Time gated plume imaging and microscopy measurements have been used to study the plasma composition and the deposition of thin carbon films. The multi-component structure of the plume emission is rationalized in terms of charge state, ions temperature and neutrals temperature. A special regard is given to the ion acceleration process occurring inside the plasma due to the high electrical field generated in the non-equilibrium plasma conditions. The use of nanosecond laser pulses, at fluences below 10 J/cm², produces interesting C-atomic emission effects, as a high ablation yield, a high fractional ionization of the plasma and presence of nanostructures deposited on near substrates.     

脉冲激光诱导Cu靶产生发光羽的特性分析

通过在不同的环境气压下拍摄脉冲激光烧蚀金属Cu诱导产生的发光羽,获取了不同区域具有不同颜色特征的发光羽照片.结果发现:发光羽的颜色随环境气压的改变而变化.采用空间分辨光谱技术,测定了激光诱导金属Cu靶产生发光羽辐射强度的空间分布,以及不同烧蚀环境气压对发光羽辐射强度的影响.研究了脉冲激光烧蚀Cu表面诱导发光的动力学过程,建立了可能的发光羽分区模型,对发光羽的不同区域发光粒子的激发机理进行了探讨,并用之定性地解释了所观察的实验现象.结果分析表明:脉冲激光诱导Cu产生的发光羽可以分为三个区域,不同区域的发光机理不同,Cu原子和Cu离子的激发机理不完全相同.     

Modeling of plume dynamics with shielding in laser ablation of carbon

The process of laser ablation of carbon in presence of background gas is simulated numerically. The plume dynamics in laser ablation is important to study for many reasons including temperature of plume particles and shielding of target by previously ablated plumes. Shielding leads directly to the change in energy deposition of incident laser pulse at the target surface and in turn influences the ablation dynamics and amount of material removed. Carbon ablation is studied for single and multiple laser hits typical for synthesis of nanotubes. Two models of correction of ablated velocity and pressure resulting from shielding effect are proposed and investigated. Numerical modeling of this plume dynamics and its integral effect of shielding is challenging due to inherent high nonlinearity of the problem. Some of available numerical techniques handles nonlinearity but are dissipative, e.g. Godunov type schemes. Other techniques are less dissipative but fail to account for strong nonlinearity typical for initial stages of ablation, e.g. the ENO-Roe. To effectively model this highly nonlinear plume dynamics a combination of two of above mentioned schemes is developed so as the numerical evaluation of fluxes is close to their physical values and the scheme has minimum dissipation. The non-monotonic behavior of ablated mass as a function of time duration between two laser pulses is studied.     

Double-peak droplet mass distribution observed during sub-ps laser ablation of Si targets

The angular distribution of the ablated material was studied during sub-ps Si laser ablation deposition using a special hemicylindrical substrate holder and different laser fluences ranging between 0.4 and 1.7 J/cm². Scanning electron microscopy analysis of the deposited films showed that, independent of the fluence, the distribution of the deposited droplets presents two maxima. The first maximum corresponds to the average plume deflection angle value due to the local surface orientation produced by the preferential etching process. The second maximum is observed approximately at 45° with respect to the normal of the target surface, and is related to the phase explosion products that expand along the incident laser beam direction. The investigation of the twofold distribution of the sub-μm size deposited droplets is important to improve the quality of the deposited coatings. PACS 81.15.Fg; 68.55.Jk; 79.20.Ds     

Characteristics of the plume particles removed by a swirling flow nozzle in laser ablation

The plume particles removed by a swirling flow nozzle in laser ablation have been characterized with numerical and experimental approaches in this paper. The swirling flow was simulated by a computational fluid dynamic (CFD) software with RNG k–ε turbulent model. The air flow passed through a specifically designed swirling flow nozzle and impinged on the substrate with various inlet velocities. The trajectories of the plume particles with various diameters in the flow field were calculated and compared with the flow visualization in the experiments. The results show that the velocity distribution of the swirling flow on the substrate was significantly affected by the swirling strength of the flow. It shows that the plasma plume was removed efficiently and the surface roughness was significantly reduced by the implementation of swirling flow in laser ablation.     

The influence of wavelength,temporal sequencing,and pulse duration on resonant infrared matrix-assisted laser processing of polymer films

We have carried out a systematic investigation of laser ablation plume interactions in resonant infrared matrix-assisted pulsed laser evaporation. The laser source utilized in this study was a mid-infrared OPO capable of dual sequential ns pulses with adjustable delay ranging from 1 to 100 μs. This unique capability enabled us both to probe the ablation plume with a second laser pulse, and to effectively double the laser fluence. The primary ablation target used for this study consisted of poly(methyl methacrylate) dissolved in a binary mixture of methanol and toluene. Both the critical thermodynamic and optical properties of the binary mixture were determined and used to interpret our results. We found that deposition rates associated with single pulse irradiation tracks with the optical absorption coefficient in the spectral range from 2,700 to 3,800 nm. In the case of dual sequential pulses, discrepancies in this trend have been linked to the rate of change in the optical absorption coefficient with temperature. The influence of fluence on deposition rate was found to follow a sigmoidal dependence. Surface roughness was observed to have a diametrically opposed trend with pulse delay depending on whether the OH or CH vibrational mode was excited. In the case of CH excitation, we suggest that the rougher films are due to the absorbance of the second pulse by droplets within the plume containing residual solvent which leads to the formation of molecular balloons and hence irregularly shaped features on the substrate.     

偏振态对飞秒激光加工石英玻璃表面质量的影响

为研究线偏振和圆偏振对飞秒激光烧蚀加工石英玻璃表面质量的影响,开展不同扫描速度的线烧蚀试验和不同线重叠率的面烧蚀试验。研究了线、圆偏振光对烧蚀线宽度的影响,利用光学显微镜和环境扫描电子显微镜观察烧蚀形貌,并使用三维表面轮廓仪进行烧蚀面粗糙度分析。结果表明:线偏振光烧蚀线宽度大于圆偏振光,且激光功率越大,线宽差异越明显;当线重叠率在65%~90%时,线偏振光烧蚀表面粗糙度随重叠率增大而增大,在重叠率为65%时达到1.33μm;线轮廓算术平均偏差随重叠率增大先减小后增大,并在重叠率为80%时达到较小值1.05μm;当重叠率不到80%时,线偏振光烧蚀面线轮廓算术平均偏差比圆偏振光小;重叠率为90%时,其线轮廓算术平均偏差反而比圆偏振光大。     

High repetition rate laser ablation for vapor–liquid–solid nanowire growth

A high repetition rate (500 kHz) solid state laser was used for the ablation process in a Pulsed Laser Deposition (PLD)/Vapor–Liquid–Solid (VLS) growing. A ZnO target was ablated with laser powers between 0.6 W and 1.2 W, and a variable number of pulses per train and trains frequencies. ZnO structures were grown on gold patterned and unpatterned substrates surfaces. Enhanced growth of the nanostructures could be noticed on the catalyst patterned surfaces. Better nanowire morphologies were also observed for bigger number of laser pulses per train. The enhancements are more evident for low laser powers. Based on plume expansion investigations, by using a high speed camera and a Particle-In-Cell (PIC) Monte-Carlo based simulations, the nanostructure morphology variations could be understood on the basis of the plume particles diffusion process and thin film versus VLS growing competition.     

Femtosecond pulsed-laser deposition of BaTiO<Subscript>3</Subscript>

The elemental composition and the surface morphology of thin films grown by laser ablation of barium titanate with femtosecond pulses at 620 nm laser wavelength have been systematically studied according to the experimental pulsed-laser deposition parameters : laser energy density, oxygen pressure, substrate temperature, target–substrate distance and substrate position (in- and off-axis geometry). Firstly, even at high temperature (700 °C), the deposits consist of coalesced particles up to 1-μm in size, mixed in a poorly crystallised tetragonal BaTiO₃ thin film. The particles formed in femtosecond pulsed-laser deposition induce a high surface roughness, which is observed whatever the experimental growth conditions and does not correspond to the droplets often observed during laser ablation in the nanosecond regime. As shown by plasma expansion dynamics, these particles propagate toward the substrate in the plasma plume with a low velocity, and are assumed to be produced by gas-phase reactions. Moreover, the cationic concentration evaluated through the Ba/Ti ratio strongly depends on the oxygen pressure in the ablation chamber and the angular position of the substrate along the normal to the target at laser impact. Indeed, the films appear to be enriched in the heavy element (Ba) when the substrate is located at high angular deviation. This fact is correlated to an increase in the lighter species (i.e. Ti) in the central part of the plasma plume. Received: 30 April 2002 / Accepted: 26 August 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +33-1/4354-2878, E-mail: millon@gps.jussieu.fr RID="**" ID="**"Also at: LSMCL, Université de Metz, 57078 Metz Cedex 3, France     

Laser irradiation effects on gold

Investigations on the laser irradiation effects on gold are explored in terms of plasma-plume dynamics and morphological and crystallographic changes. Annealed 4N gold samples were irradiated with a Q-switched Nd:YAG laser (53 mJ, 21 MW, 532 nm, and pulse width 6–8 ns) for plume dynamics using 10-ns gated fast photography. A Q-switched pulsed Nd:YAG laser (10 mJ, 1.1 MW, 1064 nm, and pulse width 9 ns) was used to irradiate the surface of the samples for morphological and crystallographic studies of laser-irradiated gold in a vacuum ～10^?3 Torr. The annealed samples were exposed to 50 shots of a Nd:YAG laser (10 mJ, 1.1 MW, 1064 nm, and pulse width 9 ns). The investigation on the plume was done by using an intensified charged-couple device ICCD-5760/IR-UV camera. The morphological investigation of the irradiated surface was carried out by analyzing micrographs obtained using an Hitachi S 3000 H scanning-electron microscope (SEM). The crystallographic studies of the irradiated samples were performed by analyzing the XRD patterns obtained using an X’ Pert Pro Pan Analytical X-ray diffractometer. The investigation on gated ICCD images of the plume reveal that, at very earlier times, the plasma-plume expansion has a linear trend, whereas, at later times, the plasma-plume expansion is nonuniform. SEM micrographs exhibit the primary mechanisms of pulsed-laser ablation (PLA), such as hydrodynamic sputtering, thermal sputtering, exfoliation sputtering, and splashing. The surface morphology was explained in terms of crater formation, swelling, burning, nucleation, grain growth, and nonsymmetric heat conduction. The nonuniform thermal expansion of gold due to thermal-energy transfer is also studied by SEM micrographs, which was supported by XRD analysis. The structural analysis on the basis of XRD shows that the composition of the irradiated samples is not disturbed even after laser irradiation. The grain sizes also changed due to laser irradiation.     

Nonstationary heating during VUV photochemical ablation of polymers

According to a previously developed pure photochemical model of VUV laser ablation of polymers, the velocity of ablation front is proportional to surface intensity, and a stationary value of the surface temperature does not depend on laser intensity. Previous estimations show, however, that this stationary surface temperature could be too high to be relevant to the photochemical mechanism. This raises a question of whether the stationary value of the surface temperature can be achieved for a given time shape of light intensity coming to the surface irradiated by a laser pulse of high enough fluence. The intensity time shape is connected not only with the time shape of a laser pulse but also with screening of laser radiation by the plume. This problem is discussed in the present communication. Specifically, it is shown that with a hyperbolic surface intensity time shape, heat diffusion can successfully compete with laser heating decreasing maximum surface temperature compared to its stationary value. The hyperbolic surface laser intensity corresponds to a rectangular laser pulse screened by plume during the photochemical ablation. This allows one to estimate that the photochemical model for a multiple-pulse VUV laser ablation with a high plume extinction coefficient is self-consistent even for a high value of stationary temperature and for high enough laser fluences. PACS 42.62.-b; 44.05.+e; 82.53.-k     

Synthesis of CaWO<Subscript>4</Subscript> nanocolloidal suspension via pulsed laser ablation and its optical properties

Pulsed laser ablation (PLA) in the liquid phase was successfully employed to synthesize calcium tungstate (CaWO₄) nanocolloidal suspension. The crystalline phase, particle morphology and laser ablation mechanism for the colloidal nanoparticles were investigated using XRD, TEM and SEM. The obtained colloidal suspension consisted of well-dispersed CaWO₄ nanoparticles which showed a spherical shape with sizes ranging from 5 to 30 nm. The laser ablation and the nanoparticle forming process were discussed under consideration of the photo-ablation mechanism, where the nanoparticles were generated by rapid condensation of the plume in high pressured ethanol vapor. The optical properties of the prepared CaWO₄ colloidal nanoparticles were analyzed in detail using XPS, Raman spectroscopy, UV-Vis spectroscopy and PL spectrophotometry. The optical band gap was estimated by Tauc and Menths law. PACS 42.62.-b; 82.70.Dd; 78.55.Hx; 81.07.Wx     

基于双相延迟模型的飞秒激光烧蚀金属模型

为了分析飞秒激光烧蚀过程,在双相延迟模型的基础上建立了双曲型热传导模型.模型中考虑了靶材的加热、蒸发和相爆炸,还考虑了等离子体羽流的形成和膨胀及其与入射激光的相互作用,以及光学和热物性参数随温度的变化.研究结果表明:等离子体屏蔽对飞秒激光烧蚀过程有重要的影响,特别是在激光能量密度较高时;两个延迟时间的比值对飞秒激光烧蚀过程中靶材的温度特性和烧蚀深度有较大的影响;飞秒激光烧蚀机制主要以相爆炸为主.飞秒激光烧蚀的热影响区域较小,而且热影响区域的大小受激光能量密度的影响较小.计算结果与文献中实验结果的对比表明基于双相延迟模型的飞秒激光烧蚀模型能有效对飞秒激光烧蚀过程进行模拟.     

Comparison of plume expansion in femtosecond laser ablation on oxidized and non-oxidized Sm surfaces

Time development of Sm⁺ and Sm ablation plume produced by the femtosecond laser irradiation has been investigated. The two-dimensional spatial profiles of Sm and Sm⁺ emitted from oxidized and non-oxidized Sm surface were visualized using a planar laser-induced fluorescence method. It was observed that the flow velocity of Sm⁺ is much faster than that of Sm plume in both surfaces. The plumes from the oxidized Sm surface show higher velocity than that from non-oxidized surface, which is originated by the small electric conductivity at the surface. Expansion property observed for Sm⁺ and Sm plume in the oxidized Sm surface ablation implies the formation of the Knundsen layer nearby the surface. Meanwhile, continuous emission of Sm indicates the large contribution of heating effect to emission process at the non-oxidized surface. We conclude that the fsLA process strongly depends on the electric property of the ablated surface and the heating effect contributes to the particle emission process on the conductive material surface.