Laser ablation of silicon and copper targets. Experimental and finite elements studies

The ablation process induced by excimer lasers is a collective phenomenon that basically involves two phenomena: the laser radiation–matter interaction and the dynamic of the ablation plume. The laser parameters, the thermal and optical properties of the material, and the surface morphology are critical factors in the ablation mechanisms affecting the direction of the ablation plume expansion. In this study, the role of the surface roughness and the evolution of its morphology under the laser irradiation were investigated. Assuming a thermal ablation model, a theoretical study of the initial steps of the laser ablation process by a finite element method using ANSYS (6.1) was performed. Different ablation experiments were carried out on silicon and copper targets using a XeCl laser. The target surface morphology changes were observed by SEM and the plume deflection was recorded by a digital camera. An acceptable agreement between the experimental and simulated results was found. This study contributes to a better understanding of the physical processes involved in the laser ablation and the relations between the plume deflection angle and the surface roughness. PACS 79.20.Ds; 81.40.Gh; 44.05.+e     

Mechanisms of ablation-rate decrease in multiple-pulse laser ablation

We present two sets of experimental results on the ablation-rate decrease with increase of the number of consecutive laser pulses hitting the same spot on the target surface. We have studied laser ablation of a carbon target with nanosecond pulses in two different interaction regimes: one with a XeCl laser (λ=308 nm) and the other with a Nd:YAG laser (λ=1064 nm), in both cases at the intensity ∼5×10⁸ W/cm² Two different mechanisms were found to be responsible for the ablation-rate decrease; they are directly related to the two different laser–matter interaction regimes. The UV-laser interaction is in the regime of transparent vapour (surface absorption). The increase of the neutral vapour density in the crater produced by the preceding laser pulses is the main reason for the decrease of ablation rate. With the IR laser each single laser pulse interacts with a partially ionised plume. With increase of the number of pulses hitting the same spot on the target surface, the laser–matter interaction regime gradually changes from the near-surface absorption to the volume absorption, resulting in the decrease in absorption in the target and thus in the decrease in the ablation rate. The change in the evaporation rate was considered for both vacuum and reactive-gas environments. Received: 21 February 2001 / Accepted: 26 February 2001 / Published online: 23 May 2001     

Picosecond and femtosecond pulsed laser ablation and deposition of quasicrystals

A Nd:glass laser with pulse duration of 250 fs and 1.3 ps has been used to evaporate a Al₆₅Cu₂₃Fe₁₂ quasicrystalline target. The gaseous phase obtained from the ablation process has been characterised by several techniques such as emission spectroscopy, quadrupole mass spectrometry and ICCD imaging, used to study the plume composition, energy and morphology. The results show that the ablation processes in the short-pulse regimes are very different to the nanosecond one. In particular the plume angular distribution shows a characteristic high cosine exponent and the composition is completely stoichiometric and independent from the laser fluence. Furthermore the mass spectra indicate the presence of clusters, both neutral and ionised and the emission from the target suggest a rapid thermalisation leading to the melting of the surface. To clarify the ablation process some films have been deposited, on oriented silicon, at different experimental conditions and analysed by scanning electron microscopy, atomic force microscopy, energy dispersive X-ray analysis and X-ray diffraction. The analyses show the presence of nanostructured films retaining the target stoichiometry but consisting of different crystalline and non crystalline phases. In particular the nanostructure supports the hypothesis of the melting of the target during the ablation and a mechanism of material ejection is proposed for both picosecond and femtosecond regimes.     

A model of nanosecond laser ablation of compound semiconductors accounting for non-congruent vaporization

We report a model of nanosecond laser ablation of compound semiconductors taking into account stoichiometry loss as a result of different volatilities of the material components. The model is based on the heat-flow equation for the bulk material and the diffusion equation for its atomic constituents and takes into account variations of material properties as functions of temperature and composition. Changing the optical response which results from stoichiometry violation is described within the concept of an effective medium and a multi-layer reflection model is applied. For cadmium telluride, as an example, the processes of ablation, melting, and resolidification under the action of a KrF laser have been studied in dynamics for particular experimental conditions in a wide range of laser fluences from the ablation threshold to the plasma shielding regimes described by the effective plasma plume representation. Multi-shot irradiation regimes have been investigated and the mechanism of the irradiation-controlled stoichiometry reversal has been elucidated.     

Hydrodynamic modeling of femtosecond laser ablation of metals in vacuum and in liquid

We numerically examine the mechanisms involved in nanoparticle formation by laser ablation of metallic targets in vacuum and in liquid. We consider the very early ablation stage providing initial conditions for much longer plume expansion processes. In the case of ultrashort laser ablation, the initial population of primary nanoparticles is formed at this stage. When a liquid is present, the dynamics of the laser plume expansion differs from that in vacuum. Low compressibility of the ambient liquid results in strong confinement conditions. As a result, ablation threshold rises drastically, the ablated material is compressed, part of it becomes supersaturated and the backscattered material additionally heats the target. The extension of a molten layer leads to the additional ablation at a later stage also favoring nanoparticle formation. The obtained results thus explain recent experimental findings and help to predict the role of the experimental parameters. The performed analysis indicates ways of a control over nanoparticle synthesis.     

Theoretical determination of the ablation rate of metals in multiple-nanosecond laser pulses irradiation regime

A detailed understanding of the physical determinants of the ablation rate in multiple nanosecond laser pulses regime is of key importance for technological applications such as patterning and pulsed-laser deposition. Here, theoretical modeling is employed to investigate the ablation of thick metallic plates by intense, multiple nanosecond laser pulses. A new photo-thermal model is proposed, in which the complex phenomena associated to the ablation process are accounted for as supplementary terms of the classical heat equation. The pulsed laser ablation in the nanosecond regime is considered as a competition between thermal vapourization and melt ejection under the action of the plasma recoil pressure. Computer simulations using the photo-thermal model presented here and the comparison of the theoretical results with experiment indicate two different mechanisms that contribute to the decrease of the ablation efficiency. First, during the ablation process the vapour/plasma plume expanding above the irradiated target attenuates the laser beam that reaches the sample, leading to a marked decrease of the ablation efficiency. Additional attenuation of the laser beam incident on the sample is produced due to the heating of the plasma by the absorption of the laser beam into the plasma plume. The second mechanism by which the ablation efficiency decreases consists of the reduction of the incident laser intensity with the lateral area, and of the melt ejection velocity with the depth of the hole.     

Mechanisms of small clusters production by short and ultra-short laser ablation

The mechanisms involved into the formation of clusters by pulsed laser ablation are studied both numerically and experimentally. To facilitate the model validation by comparison with experimental results, the time and length scales of the simulation are considerably increased. This increase is achieved by using a combination of molecular dynamics (MD) and the direct simulation Monte Carlo (DSMC) methods. The combined MD-DSMC model is then used to compare the relative contribution of the two channels of the cluster production by laser ablation: (i) direct cluster ejection upon the laser-material interaction, and (ii) collisional sticking and aggregation in the ablated gas flow. Calculation results demonstrate that both of these mechanisms play a role. The initial cluster ejection provides cluster precursors thus eliminating the three-body collision bottleneck in the cluster growth process. The presence of clusters thus facilitates the following collisional condensation and evaporation processes. The rates of these processes become considerable, leading to the modification of not only the plume cluster composition, but also the dynamics of the plume expansion. Calculation results explain several recent experimental findings.     

Impact of open de-ionized water thin film laminar immersion on the liquid-immersed ablation threshold and ablation rate of features machined by KrF excimer laser ablation of bisphenol A polycarbonate

Debris control and surface quality are potential major benefits of sample liquid immersion when laser micromachining; however, the use of an immersion technique potentially modifies the ablation mechanism when compared to an ambient air interaction. To investigate the machining characteristics, bisphenol A polycarbonate has been laser machined in air and under a controllable open liquid film. To provide quantitative analysis, ablation threshold, ablation rate and the attenuation coefficient of the immersing de-ionized (DI) water fluid were measured. In ambient air the threshold fluence was measured to be 37 mJ cm⁻². Thin film immersion displayed two trends: threshold fluences of 58.6 and 83.9 mJ cm⁻². The attenuation of DI water was found to be negligible; thus, the change in ablation rate resulted from increased confinement of the vapour plume by the liquid medium, generating higher Bremsstrahlung attenuation of the beam, lowering the laser etch rate. Simultaneously, splashing motivated by the confined ablation plume allowed release of plume pressure before plume etching commenced. This contributed to the loss of total etching efficiency. Two interaction scenarios were obsereved as a result of splashing: (i) intermediate threshold fluence, where splashing occured after every pulse in a mode that interrupted the flow entirely, leaving an ambient air interaction for the following pulse; (ii) high threshold fluence, where splashing occured for every pulse in a mode that allowed the flow to recommence over the image before the next pulse causing every pulse to experience Bremsstrahlung attenuation. Since attenuation of the immersion liquid was negligible, it is the action of the constrained ablation plume within a thin flowing immersion liquid, the resultant Bremsstrahlung attenuation and splashing events that are the critical mechanisms that modify the primary ablation characteristics.     

Femtosecond laser ablation of silicon in air and vacuum

Femtosecond(fs) pulse laser ablation of silicon targets in air and in vacuum is investigated using a timeresolved shadowgraphic method. The observed dynamic process of the fs laser ablation of silicon in air is significantly different from that in vacuum. Similar to the ablation of metallic targets,while the shock wave front and a series of nearly concentric and semicircular stripes,as well as the contact front,are clearly identifiable in the process of ablation under 1×10 5 Pa,these phenomena are no longer observed when the ablation takes place in vacuum. Although the ambient air around the target strongly affects the evolution of the ablation plume,the three rounds of material ejection clearly observed in the shadowgraphs of fs laser ablation in standard air can also be distinguished in the process of ablation in vacuum. It is proven that the three rounds of material ejection are caused by different ablation mechanisms.     

激光烧蚀聚甲醛的热-化学耦合模型及其验证

针对激光辐照聚甲醛的烧蚀现象,建立了一种包含升温、相变、热解及热解产物飞散等过程的热-化学耦合模型.采用无规热解模型描述聚甲醛升温后的热解过程,给出了不同热解率下热解产物的组成.利用基团贡献法计算烧蚀产物组分的热力学性质,并按照混合法则确定烧蚀产物混合物的名义标准沸点和临界温度.当烧蚀产物温度低于临界温度时,以液态蒸发机理表征热解产物的烧蚀,用Knudsen层关系式计算烧蚀质量;反之热解产物飞散由气体动力学机理控制,采用间断守恒关系及Jouguet条件描述烧蚀进程.本模型可给出激光辐照下聚甲醛的烧蚀质量、烧蚀温度、烧蚀产物组成和不同机理的烧蚀比率.与实验结果对比表明,当激光能量密度小于30 J/cm2时本模型能准确地描述烧蚀过程.     

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     

Dynamics of the ejected material in ultra-short laser ablation of metals

A molecular dynamics model is applied to study the formation and the early stages of ejection of material in ultra-short laser ablation of metals in vacuum. Simulations of the ablation process for iron at a pulse duration of 0.1 ps and at different laser fluences are performed. Different features of the ejection mechanism are observed below, near, and above the ablation threshold. The last is estimated as approximately 0.1 J/cm². The structure of the ablated material is found to depend on the applied laser fluence. The expanded plume consists mainly of large clusters at fluences near to the threshold. With the increase of the laser fluence the presence of the large clusters decreases. Clear spatial segregation of species with different sizes is observed in the direction normal to the surface several tens of picoseconds after the laser pulse onset. The angular distribution of the ejected material is estimated for different regimes of material removal. Above the ablation threshold the distribution is forward peaking. PACS 79.20.Ds; 52.38.Mf; 02.70.Ns; 81.05.Bx     

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利用时空分辨的测量技术,测定了XeCl紫外激光烧蚀金属Cu消融粒子的发射光谱随时间与空间的强度分布。通过在不同的氢气压强下拍摄到的XeCl308nm紫外激光烧蚀金属Cu消融粒子的发光羽照片,发现激光消融粒子发光羽的颜色在不同区域有不同的颜色,不同区域的发光羽颜色随环境气压的改变而变化。随环境气压的增大,发光羽不仅逐渐变小,而且逐渐变淡。对激光消融粒子发光羽的机理进行了探讨,激光消融粒子发光羽的发光动力学模式在不同区域有不同的发光模式,且随环境气压的变化而改变。定性地解释了所观察的实验现象。     

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.     

Subpicosecond laser ablation of copper and fused silica: Initiation threshold and plasma expansion

We investigated the subpicosecond laser ablation of copper and fused silica under 100 fs laser irradiation at 800 nm in vacuum by means of fast plume imaging and time- and space-resolved optical emission spectroscopy. We found that, to the difference of copper ablation, the laser-generated plasma from a fused silica target exhibited one “main” component only. The “slow” plasma component, observed during copper ablation and usually assigned to optical emission from nanoparticles was not detected by either plasma fast imaging or optical emission spectroscopy even when fused silica targets were submitted to the highest incident fluences used in our experiments. The characteristic expansion velocity of this unique component was about three times larger than the velocity of the fast plume component observed during copper ablation. The dependence of laser fluence on both plasma expansion and ablation rate was investigated and discussed in terms of ablation efficiency and initiation mechanisms.     

Investigation of nanoparticle generation during femtosecond laser ablation of metals

The production of nanoparticles via femtosecond laser ablation of gold and copper is investigated experimentally involving measurements of the ablated mass, plasma diagnostics, and analysis of the nanoparticle size distribution. The targets were irradiated under vacuum with a spot of uniform energy distribution. Only a few laser pulses were applied to each irradiation site to make sure that the plume expansion dynamics were not altered by the depth of the laser-produced crater. Under these conditions, the size distribution of nanoparticles does not exhibit a maximum and the particle abundance monotonously decreases with size. Furthermore, the results indicate that two populations of nanoparticles exist within the plume: small clusters that are more abundant in the fast frontal plume component and larger particles that are located mostly at the back. It is shown that the ablation efficiency is strongly related to the presence of nanoparticles in the plume.     

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.     

Angular distributions of plume components in ultrafast laser ablation of metal targets

In view of its fundamental interest and relevance to nanoparticle film production, we have characterised the nanoparticle component of the ablation plume generated in femtosecond laser irradiation of metals. The results are compared to those of the ion plume, which is considered as representative of the atomic component. At moderate laser fluences, the angular distributions of both nanoparticle and ionic components were studied by measuring the spatial distribution of deposition on a transparent substrate and with a planar Langmuir probe, respectively. Our results show that both angular profiles of the plume components can be described by Anisimov model of isentropic expansion. As the laser fluence is increased above a value of several times the ablation threshold, the shape of the nanoparticle angular distribution progressively differs from the Anisimov prediction, contrary to what is observed for the ion component. This effect is interpreted in terms of the influence of the pressure exerted by the nascent atomic plasma plume on the initial hydrodynamic evolution of nanoparticle material.