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.     

Simulation of dynamics of phase transitions in CdTe by pulsed laser irradiation

Numerical simulation of melting and solidification processes induced in CdTe by nanosecond radiation of ruby laser (λ = 694 nm, τ = 20 and 80 ns) and KrF excimer laser (λ = 248 nm, τ = 20 ns) taking into account components diffusion in melt and their evaporation from the surface has been carried out. Cd atoms evaporation has shown to essentially affect the dynamics of phase transitions in the near-surface region. Thus, in the case of the influence of ruby laser irradiation intensive surface cooling results in the formation of nonmonotone temperature profile with maximum temperature in semiconductor volume at the distance of ∼20 nm from the surface. The melt formed under the surface extends both to the surface and to the semiconductor volume as well. As a result of cadmium telluride components evaporation and diffusion in the melt the near-surface region is enriched with tellurium. The obtained melting threshold value of irradiation energy density is in a reasonable agreement with experimental data.     

Mechanisms of melt droplets and solid-particle ejection from a target surface by pulsed laser action

We suggest an explanation of the effect of melt droplets and solid particle ejection from a target surface under the impact of laser radiation with intensity 10⁸–10¹⁰ W/cm². We consider the capillary wave instabilities on the evaporating surface of melt, which lead to growth of large-scale surface structures and ejection of macroparticles. The instability increments and characteristic droplet sizes are determined. Conditions are found for droplet-free evaporation in terms of the dynamic pressure of evaporated matter.     

Flight range of the particulate in a laser-plasma generated soft X-ray chamber

Some closed expressions for the flight ranges of the spherical particle ejected from a laser-produced plasma target in buffer gas are given as a function of its initial velocity, diameter, and some parameters of the properties for gas and particle material. It is shown that when estimating the ranges of the particulates generated from the laser target, the decline of viscosity with the decrease of the gas pressure has to be considered. Received: 3 March 2000 / Accepted: 28 March 2000 / Published online: 5 July 2000     

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.     

Laser-produced iron nitrides seen by Mössbauer spectroscopy

Mössbauer spectroscopy is a very powerful tool to investigate technological processes performed mainly at the surface of materials. Nitriding of metals and steel is well established in surface engineering, and gas nitriding is used most frequently. Laser nitriding, i.e. the nitrogen take-up from the ambient gas upon irradiation of a steel surface with short laser pulses, is presented in its application to iron, stainless steel and plain carbon steels. It will be demonstrated how Mössbauer spectroscopy in combination with complementary methods (Rutherford backscattering spectroscopy, Resonant nuclear reaction analysis, Nanoindentation) can help to reveal basic mechanisms in these processes.     

Effects of post-desorption collisions on the energy distribution of SiCl molecules pulsed-laser desorbed from Cl-covered Si surfaces: Monte-Carlo simulations compared to experiments

Si surfaces covered with up to a monolayer of chlorine by exposure to a low chlorine pressure have been irradiated with nanosecond excimer-laser pulses at a fluence just large enough to melt the surface. Angle-resolved time-of-flight (TOF) distributions and surface temperatures have been measured as a function of chlorine dose between laser pulses. The TOF distributions can be fitted well by Maxwell-Boltzmann (MB) distributions for all coverages and at all desorption angles. With increasing coverage, the intensity and kinetic energy distributions become increasingly peaked along the surface normal. Monte-Carlo simulations of the effect of post-desorption collisions, occurring when many molecules are desorbed within a very short time, reproduce the experimental results quite well. It is shown that just a few collisions per molecule are sufficient to convert any initial desorption distribution into a MB one.     

Short-laser-pulse-driven emission of energetic ions into a solid target from a surface layer spalled by a laser prepulse

An efficient emission of picosecond bunches of energetic protons and carbon ions from a thin layer spalled from a organic solid by a laser prepulse is demonstrated numerically. We combine the molecular dynamics technique and multi-component collisional particle-in-cell method with plasma ionization to simulate the laser spallation and ejection of a thin (∼20–30 nm) solid layer from an organic target and its further interaction with an intense femtosecond laser pulse. In spite of its small thickness, a layer produced by laser spallation efficiently absorbs ultrashort laser pulses with the generation of hot electrons that convert their energy to ion energy. The efficiency of the conversion of the laser energy to ions can be as high as 20%, and 10% to MeV ions. A transient electrostatic field created between the layer and surface of the target is up to 10 GV/cm. Received: 13 March 2001 / Accepted: 20 March 2001 / Published online: 20 June 2001     

Time-resolved investigations of plasma and melt ejections in?metals by pump-probe shadowgrpahy

Ablation of bulk metals (Al, Cu) has been investigated in situ by means of high-resolution pump-probe photography using pump laser radiation of pulse duration t _p=80 fs, at wavelength of 820 nm. Depending on material-specific parameters, qualitatively different ablation phenomena have been observed. Structural analysis by electron and optical microscopies reveals rosette-like surface structures showing the morphology of the ablated regions. The temporal development of the ablation dynamics can be conditionally categorized into different characteristic time regions. Particularly, laser induced melt injection has been observed in the time range of 700 ns to 1.1 μs after the initial laser-metal interaction.     

Simulation of composition modification in ZnSe by nanosecond radiation of excimer laser

A numerical simulation of the composition modification induced in ZnSe by nanosecond irradiation of the KrF excimer laser (λ = 248 nm, τ = 20 ns) has been carried out. Intensive evaporation of components has shown to results in the material surface cooling and forming a nonmonotone temperature profile with maximum temperature in semiconductor volume at the distance of ∼6 nm from the surface. As a result of evaporation and diffusion of components formation of the near-surface layer with nonstoichiometric composition takes place and enrichment of selenium reaches maximum value not on the surface, but in the semiconductor volume.     

Experimental and numerical study of surface alloying by femtosecond laser radiation

Here we report on experimental studies of femtosecond laser induced surface metal alloying. We demonstrate that layers of different metals can be mixed in a certain range of laser pulse energies. Numeric simulations demonstrate that the sub-surface melting and mixing is advantaged through the difference in the electron-phonon coupling constants of the metals in the multi-layer system. Dependence of the depth of the mixed layer on the number of laser pulses per unit area is studied. Numeric simulations illustrate physical picture of the laser alloying process.     

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.     

Pulse regime in formation of fractal fibers

The pulse regime of vaporization of a bulk metal located in a buffer gas is analyzed as a method of generation of metal atoms under the action of a plasma torch or a laser beam. Subsequently these atoms are transformed into solid nanoclusters, fractal aggregates and then into fractal fibers if the growth process proceeds in an external electric field. We are guided by metals in which transitions between s and d-electrons of their atoms are possible, since these metals are used as catalysts and filters in interaction with gas flows. The resistance of metal fractal structures to a gas flow is evaluated that allows one to find optimal parameters of a fractal structure for gas flow propagation through it. The thermal regime of interaction between a plasma pulse or a laser beam and a metal surface is analyzed. It is shown that the basic energy from an external source is consumed on a bulk metal heating, and the efficiency of atom evaporation from the metal surface, that is the ratio of energy fluxes for vaporization and heating, is 10^–3–10^–4 for transient metals under consideration. A typical energy flux (~10⁶ W/cm²), a typical surface temperature (~3000 K), and a typical pulse duration (~1 μs) provide a sufficient amount of evaporated atoms to generate fractal fibers such that each molecule of a gas flow collides with the skeleton of fractal fibers many times.     

Thermal surface-tension coefficient of metals in polymolecular adsorption. Allowance for the difference in metals in the solid and liquid states

A brief survey is made of studies of the thermal coefficient of surface tension. It is shown that the coefficient should increase with the transition of a melt to the solid phase and with the adsorption of different substances on the surface of metals. The completed analysis indicates that the liquid phase has a greater adsorption capacity than the solid phase.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 10, pp. 59–63, October, 1985.     

Dynamics of the plume formation and parameters of the ejected clusters in short-pulse laser ablation

The dynamics of the early stages of the ablation plume formation and the mechanisms of cluster ejection are investigated in large-scale molecular dynamics simulations. The cluster composition of the ablation plume has a strong dependence on the irradiation conditions and is defined by the interplay of a number of processes during the ablation plume evolution. At sufficiently high laser fluences, the phase explosion of the overheated material leads to the formation of a foamy transient structure of interconnected liquid regions that subsequently decomposes into a mixture of liquid droplets, gas-phase molecules, and small clusters. The ejection of the largest droplets is attributed to the hydrodynamic motion in the vicinity of the melted surface, especially active in the regime of stress confinement. Spatially resolved analysis of the dynamics of the plume formation reveals the effect of segregation of the clusters of different sizes in the expanding plume. A relatively low density of small/medium clusters is observed in the region adjacent to the surface, where large clusters are being formed. Medium-size clusters dominate in the middle of the plume and only small clusters and monomers are observed near the front of the expanding plume. Despite being ejected from deeper under the surface, the larger clusters in the plume have substantially higher internal temperatures as compared to the smaller clusters. The cluster-size distributions can be relatively well described by a power law Y(N)∼N^-τ with exponents different for small, up to ∼15 molecules, and large clusters. The decay is much slower in the high-mass region of the distribution. Received: 13 October 2001 / Accepted: 18 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +1-434/982-5660, E-mail: lz2n@virginia.edu     

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.      

Computer simulation of graphite target ablation under the action of a nanosecond laser pulse

A quasi-gasdynamic approach is used for computer simulation of plasma expansion from a graphite plate subjected to a nanosecond laser pulse. A one-component plasma consisting of carbon molecules alone is considered. This simplifies the experimental conditions used previously to study the dynamics of the gas resulting from evaporation. The results of computer experiment conducted for different initial temperatures and pressures of the plasma are in good qualitative agreement with the real experimental data including in the time instant the density of the expanding gas reaches a maximum. It is shown that high-density clusters are likely to appear in front of the main plasma flux. The results of the computer simulation are compared with the Singh approximation of pressure, velocity, and density of the gas flow. It is concluded that this approximation is valid only within a short (compared with the entire expansion length) plasma expansion interval existing during the initial spread for t = 4 × 10^?9 s.     

Formation of microtower structures on nanosecond laser ablation of liquid metals

We report the formation of microtower structures, observed on multishot nanosecond laser irradiation of liquid metals (Ga, In, Sn–Pb alloy, Wood’s metal). Ablation in a reactive ambient gas (air, nitrogen, sulfur hexafluoride, nitrogen trifluoride) is shown to lead to a tower-like structure growing on the irradiated surface at a rate of 3–20 μm per pulse depending on laser fluence and the types of metal and ambient gas. The interplay between different processes in the heat-affected zone of the irradiated samples is analyzed, including ablation, thermal expansion, temperature variations of viscosity, surface tension, thermal stresses, capillary effects, and surface chemistry. A clear picture of microtower origin has been established, and qualitative modeling can explain the formation mechanism.     

Experimental study on reflection of high-intensity nanosecond Nd:YAG laser pulses in ablation of metals

The total reflectivity of tin and magnesium in ablation by nanosecond Nd:YAG laser pulses in air is studied. It was found that the high initial reflectivity of the studied metals undergoes a significant drop to values of 0.11 for Sn and 0.16 for Mg within a laser fluence range between about 0.8 and 11 J/cm². These reduced reflectivity values remain virtually unchanged with further increasing laser fluence. This study shows that a significant reflectivity decrease of the studied metals is caused by plasma formation in front of the irradiated surface. Below the plasma formation threshold, the reflectivity of the studied metals is observed to be virtually independent of laser fluence, indicating a small role of Drude׳s temperature effect on the reflectivity of the studied samples.