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     

纳秒激光脉冲诱导硅表面微结构

利用Nd:YAG纳秒激光脉冲,在能量密度为1～10 J/cm2范围内辐照单晶硅,形成了表面锥形微结构,在SF6气氛和空气环境下均形成了锥形尖峰表面微结构。SF6气氛下产生的锥形尖峰顶端都有小球,部分锥形上还有二次尖峰形成,空气中纳秒激光诱导的锥形尖峰微结构顶端和边缘有由液滴固化形成的粒状物质,不同于利用准分子纳秒激光诱导的细长须状结构和飞秒激光辐照下产生的具有表面枝蔓状纳米结构的锥形微结构。实验结果表明,这种尖峰微结构的形成与辐照激光的波长和脉冲持续时间有关。对空气中微构造硅的辐射反射的初步研究表明,在500～2 400 nm范围内的光辐射反射率不高于20%。     

Nanosecond pulsed laser ablation of silicon in liquids

Laser fluence and laser shot number are important parameters for pulse laser based micromachining of silicon in liquids. This paper presents laser-induced ablation of silicon in liquids of the dimethyl sulfoxide (DMSO) and the water at different applied laser fluence levels and laser shot numbers. The experimental results are conducted using 15 ns pulsed laser irradiation at 532 nm. The silicon surface morphology of the irradiated spots has an appearance as one can see in porous formation. The surface morphology exhibits a large number of cavities which indicates as bubble nucleation sites. The observed surface morphology shows that the explosive melt expulsion could be a dominant process for the laser ablation of silicon in liquids using nanosecond pulsed laser irradiation at 532 nm. Silicon surface’s ablated diameter growth was measured at different applied laser fluences and shot numbers in both liquid interfaces. A theoretical analysis suggested investigating silicon surface etching in liquid by intense multiple nanosecond laser pulses. It has been assumed that the nanosecond pulsed laser-induced silicon surface modification is due to the process of explosive melt expulsion under the action of the confined plasma-induced pressure or shock wave trapped between the silicon target and the overlying liquid. This analysis allows us to determine the effective lateral interaction zone of ablated solid target related to nanosecond pulsed laser illumination. The theoretical analysis is found in excellent agreement with the experimental measurements of silicon ablated diameter growth in the DMSO and the water interfaces. Multiple-shot laser ablation threshold of silicon is determined. Pulsed energy accumulation model is used to obtain the single-shot ablation threshold of silicon. The smaller ablation threshold value is found in the DMSO, and the incubation effect is also found to be absent.     

Drilling enhancement by nanosecond-nanosecond collinear dual-pulse laser ablation of titanium in vacuum

Laser ablation of titanium in vacuum was performed using single- and dual-pulse regime in order to study crater formation. Crater profiles were analyzed by optical microscopy. It was found that the repetition-rate plays an important role in a process of laser ablation. The drilling is most effective for the highest repetition-rate. For the same total number of laser pulses clear drilling enhancement was achieved by dual-pulse regime of ablation in comparison to single-pulse regime. The strongest ablation rate in dual-pulse regime was achieved for the delay time between the pulses τ = 370 ns. Results are discussed in terms of decreased ablation threshold due to continuous heating of the target during the experiment.     

Laser-induced breakdown spectroscopy: A versatile tool for monitoring traces in materials

Laser-induced breakdown spectroscopy (LIBS) is an emerging technique for simultaneous multi-elemental analysis of solids, liquids and gases with minute or no sample preparation and thus revolutionized the area of on-line analysis technologies. The foundation for LIBS is a solid state, short-pulsed laser that is focused on a sample to generate a high-temperature plasma, and the emitted radiation from the excited atomic and ionic fragments produced within the plasma is characteristic of the elemental composition of the sample that can be detected and analyzed using a suitable optical spectrograph. In the present paper, the applicability of LIBS for different solid samples having homogeneous (silver ornament, aluminum plate) or heterogeneous composition (soil) using nanosecond laser pulses is discussed. Nanosecond pulse laser makes plasma at the sample surface even at very low pulse energies and also allows for precise ablation of the substrate material with little damage to the surrounding area. We have also studied the penetration of different heavy metals inside the soil surface.      

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.     

Self-Injection and Acceleration of Monoenergetic Electron Beams from Laser Wakefield Accelerators in a Highly Relativistic Regime

Self-injection and acceleration of monoenergetic electron beams from laser wakefield accelerators are first investigated in the highly relativistic regime, using 100 TW class, 27 fs laser pulses. Quasi-monoenergetic multi- bunched beams with energies as high as multi-hundredMeV are observed with simultaneous measurements of side-scattering emissions that indicate the formation of self-channelfing and self-injection of electrons into a plasma wake, referred to as a ＇bubble＇. The three-dimensional particle-in-cell simulations confirmed multiple self-injection of electron bunches into the bubble and their beam acceleration with gradient of 1.5 GeV/cm.     

Impact of the lasr wavelength and fluence on the ablation rate of aluminium

The dependence of the ablation rate of aluminium on the fluence of nanosecond laser pulses with wavelengths of 532 nm and respectively 1064 nm is investigated in atmospheric air. The fluence of the pulses is varied by changing the diameter of the irradiated area at the target surface, and the wavelength is varied by using the fundamental and the second harmonic of a Q-switched Nd-YAG laser system. The results indicate an approximately logarithmic increase of the ablation rate with the fluence for ablation rates smaller than ∼6 μm/pulse at 532 nm, and 0.3 μm/pulse at 1064 nm wavelength. The significantly smaller ablation rate at 1064 nm is due to the small optical absorptivity, the strong oxidation of the aluminium target, and to the strong attenuation of the pulses into the plasma plume at this wavelength. A jump of the ablation rate is observed at the fluence threshold value, which is ∼50 J/cm² for the second harmonic, and ∼15 J/cm² for the fundamental pulses. Further increasing the fluence leads to a steep increase of the ablation rate at both wavelengths, the increase of the ablation rate being approximately exponential in the case of visible pulses. The jump of the ablation rate at the threshold fluence value is due to the transition from a normal vaporization regime to a phase explosion regime, and to the change of the dimensionality of the hydrodynamics of the plasma-plume.      

Experimental investigation of ablation efficiency and plasma expansion during femtosecond and nanosecond laser ablation of silicon

Femtosecond laser (Ti:sapphire, 100 fs pulse duration) ablation of silicon in air was compared with nanosecond laser (Nd:YAG, 3 ns pulse duration) ablation at ultraviolet wavelength (266 nm). Laser ablation efficiency was studied by measuring crater depth as a function of pulse number. For the same number of laser pulses, the fs-ablated crater was about two times deeper than the ns-crater. The temperature and electron number density of the laser-induced plasma were determined from spectroscopic measurements. The electron number density and temperature of fs-induced plasmas decreased faster than ns-induced plasmas due to different energy deposition mechanisms. Images of the laser-induced plasma were obtained with femtosecond time-resolved laser shadowgraph imaging. Plasma expansion in both the perpendicular and the lateral directions were compared. PACS 52.38.Mf; 52.30.-q     

纳秒紫外重复脉冲激光烧蚀单晶硅的热力学过程研究

采用波长为355 nm的纳秒紫外重复脉冲激光对单晶硅片进行了盲孔加工实验, 观测了随脉冲增加激光烧蚀硅片的外观形貌和盲孔孔深、孔径的变化规律, 并对紫外激光辐照硅片的热力学过程进行了分析. 研究结果表明:紫外激光加工硅盲孔是基于热、力效应共同作用的结果, 热效应会使得硅材料熔化、气化甚至发生电离产生激光等离子体,为材料的去除提供条件;激光等离子体冲击波以及高温气态物向外膨胀会对熔化材料产生压力致使其向外喷射,为重复脉冲的进一步烧蚀提供了条件;力效应主要沿着激光传输的方向,垂直于硅表面,使得去除部位主要集中在孔的深度方向,达到较高的孔径比,实验观察孔径比可达8:1;此外,激光等离子体的产生也阻止了激光对靶面的作用,加之随孔深的增加激光发生散焦,使得烧蚀深度有一定的限制,实验观察烧蚀脉冲个数在前100个时加工效率较高.     

The damage mechanism of fused silica surface induced by 355 nm nanosecond laser

In order to understand the physical mechanism, time-resolved dynamics of 355 nm nanosecond laser induced entrance and exit surface damage on fused silica was investigated by using shadow graphic technique. The results show that the damage mechanism is different between the entrance and exit surface during nanosecond laser interaction with fused silica. The plasma and shock waves in air is relatively higher at the entrance surface. The entrance surface damage is reduced because plasma shielding limits energy deposition. Without plasma shielding, the exit surface damage is more serious for more laser energy deposition in material. And without the stress of plasma and shock waves, the material is ejected easily at rear surface. These are confirmed by damage micrograph at the entrance and exit surface.     

Role of laser-induced plasma in ultradeep drilling of materials by nanosecond laser pulses

Radiative effects of the laser-induced ablative plasma on the heating and ablation dynamics of materials irradiated by nanosecond laser pulses are studied by the example of graphite ablation. On the basis of combined thermal and gas dynamic modeling, the laser-induced plasma plume is shown to be a controlling factor responsible for ultradeep laser drilling due to plasma radiation, both bremsstrahlung and recombinative. We demonstrate that plasma radiative heating of the target considerably deepens the molten layer, thus explaining the observed crater depths.     

Surface modification of a WTi thin film on Si substrate by nanosecond laser pulses

Interaction of a nanosecond transversely excited atmospheric (TEA) CO₂ laser, operating at 10.6 μm, with tungsten-titanium thin film (190 nm) deposited on silicon of n-type (1 0 0) orientation, was studied. Multi-pulse irradiation was performed in air atmosphere with laser energy densities in the range 24-49 J/cm². The energy absorbed from the laser beam was mainly converted to thermal energy, which generated a series of effects. The following morphological changes were observed: (i) partial ablation/exfoliation of the WTi thin film, (ii) partial modification of the silicon substrate with formation of polygonal grains, (iii) appearance of hydrodynamic features including nano-globules. Torch-like plumes started appearing in front of the target after several laser pulses.     

Sub-picosecond UV laser ablation of metals

Laser ablation of Nickel, Copper, Molybdenum, Indium, Tungsten and Gold by short ultraviolet laser pulses (0.5 ps, 248 nm) in vacuum is reported for the first time. For Nickel and Indium, ablation is also studied in air to demonstrate the influence of the ambient atmosphere. Metal ablation in air is significantly less efficient than in vacuum due to redeposition of ablated material. The ablation rates in vacuum are discussed using a thermal model, which also allows to estimate ablation rates for other metals from basic optical and thermal properties. A comparison of the morphology of ablation sites after nanosecond and sub-picosecond ablation shows unequivocally the advantages of short-pulse laser ablation for high-precision patterning of thermally good conducting materials in micron-scale dimensions.     

Formation of linear momentum in a rod during a laser pulse–matter interaction

Recently, we developed an optodynamic experimental technique that makes it possible to measure the linear momentum obtained by a metal target sample in the shape of a rod during a nanosecond laser pulse interaction in the ablative regime. The height of the rod’s rear end axial step-like displacement, caused by the first reflection of the laser-generated ultrasonic wave, is proportional to the linear momentum acquired by the rod. In comparison with commonly used ballistic methods, we can determine the acquired momentum on a much shorter time scale corresponding to the wave transition time, from the front to the rear end of the rod. Using this method we investigated the ambient air pressure dependence on the formation of linear momentum over a laser intensity range, from the ablation threshold to values about ten times higher. Steel rods of various diameters were used to demonstrate the effect of an expanding blast wave which delivers additional momentum to the target, when the laser beam on the target surface is smaller than the target itself. The typical value of the acquired target momentum is on the order of μN s and 10 μN s/J for the momentum coupling coefficient.     

大气环境下飞秒激光对铝靶烧蚀过程的研究

利用时间分辨的光阴影成像技术研究了在大气环境下飞秒激光烧蚀铝靶的动态过程. 在入射激光能量为4 mJ, 激光光斑超过1 mm时, 激光烧蚀区表面物质以近似平面冲击波形式向外喷射; 在同样激光能量下、激光光斑较小时(约0.6 mm), 激光烧蚀区以近似半球型冲击波形式向外喷射. 当激光能量比较大时(7 mJ), 发现空气的电离对于激光烧蚀靶材有着重要影响. 在光轴附近烧蚀产生的喷射物具有额外的柱状和半圆型的结构, 叠加在平面冲击波结构上.     

Generation and expansion of laser-induced plasma as a spectroscopic emission source

Laser-induced plasma represents today a widespread spectroscopic emission source. It can be easily generated using compact and reliable nanosecond pulsed laser on a large variety of materials. Its application for spectrochemical analysis for example with laser-induced breakdown spectroscopy (LIBS) has become so popular that one tends to forget the complex physical and chemical processes leading to its generation and governing its evolution. The purpose of this review article is to summarize the backgrounds necessary to understand and describe the laser-induced plasma from its generation to its expansion into the ambient gas. The objective is not to go into the details of each process; there are numerous specialized papers and books for that in the literature. The goal here is to gather in a same paper the essential understanding elements needed to describe laser-induced plasma as results from a complex process. These elements can be dispersed in several related but independent fields such as laser-matter interaction, laser ablation of material, optical and thermodynamic properties of hot and ionized gas, or plasma propagation in a background gas. We believe that presenting the ensemble of understanding elements of laser-induced plasma in a comprehensive way and in limited pages of this paper will be helpful for further development and optimized use of the LIBS technique. Experimental results obtained in our laboratory are used to illustrate the studied physical processes each time such illustration becomes possible and helpful.     

激光等离子体动量转换效率的实验研究

强激光与固体靶相互作用时，产生的高速喷射的等离子体对靶具有强烈的反冲作用，因此，激光等离子体可以作为一种新型的推进动力源.与传统的化学燃料推动相比，激光等离子体具有较高的比冲和有效载荷比等特点.对纳秒激光脉冲与铝、石墨、铅和碳氢靶相互作用时，等离子体对靶的冲量进行了实验测量，研究了大气与真空环境下的靶动量与激光聚焦面积的关系，并对部分实验结果与理论计算的数值进行了比较.实验结果显示，大气与真空环境下的靶动量有很大的差异，并且真空下的靶动量受材料性质的影响较大，与以往长脉冲激光的实验结果有很大的不同. 关键词： 激光等离子体 动量 动量耦合系数     

Time-resolved spectroscopy measurements of a titanium plasma induced by nanosecond and femtosecond lasers

We have studied the plasma induced at the surface of a titanium target following irradiation with femtosecond and nanosecond laser pulses. Time-resolved imaging and spectroscopic measurements allowed us to evidence some features specific to the femtosecond-laser-induced plasma. In this ultrashort interaction regime, we could discriminate between three different velocity populations in the plasma expansion. Coulomb explosion firstly creates highly energetic Ti⁺ ions, which are followed by atomic neutral titanium and lastly by nanoscale titanium oxide clusters. Received: 28 September 2001 / Accepted: 9 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +33-1/6931-9996, E-mail: albert@ensta.fr     

Laser ablation of energetic polymer solutions: effect of viscosity and fluence on the splashing behavior

Laser plasma thrusters are a new kind of propulsion system for small satellites, and work with the thrust created by the laser ablation of a target. Liquid polymer solutions are very promising fuels for such systems, provided that no splashing of the target occurs, because ejection of droplets strongly decreases the performances of the system. We have investigated the nanosecond infrared laser ablation of glycidyl azide polymer solutions containing carbon nanoparticles as absorber. Shadowgraphy imaging revealed two cases, namely splashing regime and solid-like behavior. The transition between both regimes depends on the viscosity of the solution and on the laser fluence, and is explained by the recoil force acting on the target. Appropriate conditions to avoid splashing were identified, showing that this liquid polymer solution is a suitable fuel for laser plasma thrusters.