Energy balance of pulsed laser ablation: thermal model revised

We present the results of modeling of nanosecond laser ablation of graphite, niobium, YBa₂Cu₃O₇ superconductor, and silicon performed on the basis of a modified thermal model which includes a thorough calculation of the solid–melt interface. The model is based on experimental data on mass removal and takes into account plasma absorption. The numerical results of the laser energy balance are presented over a wide range of laser fluences. The probable critical temperatures for the materials studied have been estimated on the basis of the modeling. PACS 52.38.Mf; 79.20.Ds     

Thermal stability of amorphous carbon films deposited by pulsed laser ablation

Diamond-like carbon (DLC) films have been grown on Si substrates at ambient temperature by the pulsed-laser ablation technique, using pulses of different durations both in the nano- and picosecond ranges and at various energy fluences. The stability of these films was investigated as a function of thermal anneals performed in UHV conditions up to 1273 K. Their physico-chemical properties have been characterized by different techniques including X-ray photo-emission, Auger electron and electron-energy-loss spectroscopies, Raman scattering, spectroscopic ellipsometry and atomic-force microscopy. The thermal stability of the films has been demonstrated to be related to their initial structural (sp³/sp² ratio) and chemical (contaminant) properties. DLC layers prepared under optimized conditions have been found to show a very good thermal stability up to 900 K. Received: 4 Jule 2000 / Accepted: 6 July 2000 / Published online: 6 September 2000     

An analytical continuum-based model of time-of-flight distributions for pulsed laser ablation

An analytical model for time-of-flight (TOF) distributions of particles produced by pulsed laser ablation in vacuum has been proposed. The model takes into account the hydrodynamic expansion stage of the ablation plume and is based on a ‘sudden freeze’ model developed previously for steady-state supersonic jets. It is assumed that a continuum-like expansion of the plume takes place until a freezing time moment t _free (or, alternatively, until a ‘freezing distance’ x _free) whereupon the collisionless expansion begins. The proposed model is applied for analysis of experimental data on graphite ablation with nanosecond laser pulses. For verification, the analytical distributions are compared with calculated results obtained using a hybrid model combining a thermal model of laser-induced material heating with calculations of the plume dynamics by the direct simulation Monte Carlo (DSMC) method. It is shown that the proposed model can accurately estimate the surface temperature for conditions when the common approach fails.     

KrF pulsed laser ablation of polyimide

In the present paper, polyimide surfaces were processed with pulsed KrF laser radiation at fluences near the ablation threshold. The morphology of the processed surfaces was studied by scanning electron microscopy and chemical analyses performed by electron dispersive spectroscopy. The formation of conical structures was observed for radiation fluences lower than 0.5 J/cm². The areal density of cones increases with the number of pulses and decreases with the radiation fluence. At low fluences (<150 J/cm²), cones are formed due to shadowing by calcium phosphate impurities while for higher fluences the main mechanism of cones formation is believed to be radiation hardening.     

A simple model for high fluence ultra-short pulsed laser metal ablation

The ultra-short laser metal ablation is a very complex process, the complete simulation of which requires applications of complicated hydrodynamics or molecular dynamics models, which, however, are often time-consuming and difficult to apply. For many practical applications, where the laser ablation depth is the main concern, a simplified model that is easy to apply but at the same time can also provide reasonably accurate predictions of ablation depth is very desirable. Such a model has been developed and presented in this paper, which has been found to be applicable for laser pulse duration up to 10 ps based on comparisons of model predictions with experimental measurements.     

Interface kinetics during pulsed laser ablation

This work investigates evaporation kinetics -- the relation between the surface temperature and pressure during excimer laser ablation. Nickel targets are ablated by excimer laser pulses in a laser fluence range between 1 and 6 J/cm², with the upper limit exceeding the threshold of phase explosion (5 J/cm²). The surface pressure is determined with a polyvinylidene fluoride (PVDF) piezoelectric transducer. When phase explosion occurs, the surface temperature is known to be near the thermodynamic critical temperature, therefore, by measuring the surface pressure, the surface temperature-pressure relation is determined at the threshold fluence of phase explosion. The surface temperature and the threshold fluence of phase explosion are also estimated from the measured velocity of the vapor plume and gas dynamics calculations. It is shown that, during excimer laser ablation, the temperature and pressure relation deviates significantly from the equilibrium kinetic relation.     

Nanosecond laser ablation for pulsed laser deposition of yttria

A thermal model to describe high-power nanosecond pulsed laser ablation of yttria (Y₂O₃) has been developed. This model simulates ablation of material occurring primarily through vaporization and also accounts for attenuation of the incident laser beam in the evolving vapor plume. Theoretical estimates of process features such as time evolution of target temperature distribution, melt depth and ablation rate and their dependence on laser parameters particularly for laser fluences in the range of 6 to 30 J/cm² are investigated. Calculated maximum surface temperatures when compared with the estimated critical temperature for yttria indicate absence of explosive boiling at typical laser fluxes of 10 to 30 J/cm². Material ejection in large fragments associated with explosive boiling of the target needs to be avoided when depositing thin films via the pulsed laser deposition (PLD) technique as it leads to coatings with high residual porosity and poor compaction restricting the protective quality of such corrosion-resistant yttria coatings. Our model calculations facilitate proper selection of laser parameters to be employed for deposition of PLD yttria corrosion-resistive coatings. Such coatings have been found to be highly effective in handling and containment of liquid uranium.     

Femtosecond pulsed laser ablation with spatial filtering

With the rise in demand for miniaturized features with better acute edge acuity and negligible thermal damage zone, one of the key vital areas lies in the refinement of the quality of the laser beam itself. Spatial filter is routinely used in optical micromachining systems to smoothen the Gaussian profile of the machining spot in order to obtain a feature of the desired quality. However, its profile smoothening effect has never been investigated for femtosecond pulsed laser micromachining process since the extremely high peak power of femtosecond pulses will cause damage on the filtering aperture of spatial filter. During the development of an acousto-optical micromachining system using femtosecond pulses, we found that if the damage of the filtering aperture can be circumvented, spatial filter can improve the machining quality of femtosecond pulse ablation, especially when ablation is conducted at low-fluency range (just above the ablation threshold fluency). In this paper, we investigate and demonstrate both the improvement and potential that beam refinement can bring about. In our experiment, a series of test patterns were ablated with a 400 nm second-harmonic Ti:Sapphire femtosecond laser of 150 fs duration at varying pulse energy ranging from 31 to 39 nJ. The specimen used in the experiment is a platinum- (Pt) sputtered coating of 100 nm thickness on a quartz substrate. The results show a significant improvement in the constancy of the shape as well as the size of ablated feature, revealing an improved beam profile and beam energy distribution due to spatial filtering.     

Metal absorptivity in femtosecond pulsed laser ablation

In this paper, the effect of the absorptivity of metal on femtosecond pulsed laser ablation is investigated. The formulas for the absorptivity depending on target temperature are derived from Maxwell Equations and the Lambert-Beer’s law. Based on this, a new two-temperature model is proposed to describe the femtosecond pulsed laser ablation with metal. Then, using Au as an example, a finite difference method is employed to simulate the space-dependent and time-dependent absorptivity and the target temperature. The temperature evolution of our model is compared with the result obtained form the heat conduction model taking the absorptivity as constant. It is shown that the absorptivity plays an important role in the femtosecond pulsed laser ablation. The results of this paper are helpful in choosing the best technical parameters in femtosecond pulsed laser ablation.      

Thermal properties of 15-mol% gadolinia doped ceria thin films prepared by pulsed laser ablation

Thermal properties of 15-mol% gadolinia doped ceria thin films (Ce_0.85Gd_0.15 O_1.925) prepared by pulsed laser ablation on silicon substrates in the temperature range 473–973 K are presented. Thermal diffusivities and thermal conductivities were evaluated using photoacoustic spectroscopy. The influence of grain size on thermal properties of the films as a function of deposition temperature is studied. It is observed that the thermal diffusivity and the conductivity of these films decreases up to 873 K and then increases with substrate temperatures. The thermal properties obtained in these films are discussed on the basis of influence of grain size on phonon scattering.     

Femtosecond pulsed laser ablation of thin gold film

Laser micromachining on 1000 nm-thick gold film using femtosecond laser has been studied. The laser pulses that are used for this study are 400 nm in central wavelength, 150 fs in pulse duration, and the repetition rate is 1 kHz. Plano-concave lens with a focal length of 19 mm focuses the laser beam into a spot of 3 μm (1/e² diameter). The sample was translated at a linear speed of 400 μm/s during machining. Grooves were cut on gold thin film with laser pulses of various energies. The ablation depths were measured and plotted. There are two ablation regimes. In the first regime, the cutting is very shallow and the edges are free of molten material. While in the second regime, molten material appears and the cutting edges are contaminated. The results suggest that clean and precise microstructuring can be achieved with femtosecond pulsed laser by controlling the pulse energy in the first ablation regime.     

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.     

Femtosecond pulsed laser ablation deposition of tantalum carbide

In this work a frequency-doubled Nd:glass laser with a pulse duration of 250 fs has been used to ablate a TaC target and to deposit thin films on silicon. The results have been compared with those previously obtained by nanosecond pulsed laser deposition and evidence of large differences in the plasma characteristics has been revealed. In particular, in the femtosecond and nanosecond plumes the energy and the velocity of neutral and ionized particles are very different. The features of femtosecond ablation include the delayed emission from the target of large and slow particles. The characteristics of the femtosecond plasma are clearly related to the morphology and composition of the deposited films and the results show a nanostructure consisting of a large number of spherical particles, with a mean diameter of about 50 nm, with a stoichiometry corresponding to Ta₂C. To explain these features, an ablation-deposition mechanism, related to the ejection of hot particles from the target, is proposed.     

Enhancement of pulsed laser ablation assisted with continuous wave laser irradiation

Continuous wave(CW) laser irradiation is employed to enhance the pulsed laser ablation of silicon and stainless steel(316 L)samples. Different surface temperatures generated by the CW laser irradiation are set as the initial working circumstance for the pulsed laser ablation. The diameter and depth of laser-ablated craters are measured to study threshold fluence, pulse incubation coefficient and ablation rate under different surface temperatures. Numerical simulation employing Heat Transfer in Solid and Deformed Geometry Interface modules in COMSOL is performed to estimate ablation rate theoretically based on Hertz-Knudsen equation. The realized crater-related data are analyzed to further obtain their dependences on surface temperature. The parametric and morphological studies indicate that the weakened plasma shielding effect and thermal diffusion in the ablated region induced by the CW laser irradiation lead to the enhanced pulsed laser ablation significantly.     

A simplified predictive model for high-fluence ultra-short pulsed laser ablation of semiconductors and dielectrics

Ultra-short pulsed laser ablation is a very complicated process and a predictive model is very desirable for process design and optimization in practical applications. However, the molecular dynamics or hydrodynamic models, although they are powerful and necessary tools for the study of the fundamental physics, are time-consuming and difficult to apply for practical applications. In this paper, a predictive, simplified and easy to apply model has been developed for high-fluence ultra-short laser ablation of semiconductors and dielectrics. Unlike many other simplified models, this model does not involve any free adjustable variables. The model predictions agree well with experimental measurements for femtosecond laser ablation, while the model is not very applicable for pulse durations more than ∼10 ps.     

脉冲激光烧蚀材料等离子体反冲压力物理模型研究与应用

分析了脉冲激光烧蚀材料等离子体等温膨胀阶段的物理特性,建立了脉冲激光烧蚀材料等离子体压力三维方程与动力学模型.应用所建模型,数值分析了单脉冲激光烧蚀青铜金刚石砂轮等离子体相关特性,得到等离子体的反冲压力最大值870 Pa出现在约25 ns后,距离砂轮表面距离约0.05 mm处.相关条件下开展脉冲激光烧蚀青铜金刚石砂轮试验,采用高速相机观测烧蚀砂轮过程中的飞溅现象;采用光栅光谱仪测量等离子体空间发射光谱,计算了等离子体电子温度、电子密度以及反冲压力.实验表明脉冲激光烧蚀青铜金刚石砂轮等离子体反冲压力可以不计,同时也验证了气体方程与动力学模型的正确性和可行性,对脉冲光纤激光烧蚀工艺优化具有启示意义.     

Plume separation effect in pulsed laser ablation deposition

The results of a new geometrical configuration of pulsed laser ablation deposition technique that uses a hemi-cylindrical transparent plastic substrate are presented and discussed. With the new arrangement, two distinct components with different material compositions have been clearly observed. While the first component comprises atoms, ions and molecules and constitutes visible or the so-called luminous plume, the second component is formed of fragments, clusters and liquid droplets and is invisible to the naked eye. The latter component constitutes a major part of the ablated material. The luminous plume symmetry axis does not coincide with the mass distribution symmetry axis. In the case of Si ablation and 45° incident beam angle, the maximum deflection angle of the luminous plume reaches 30° with respect to the normal to the target surface, while the deflection angle of the second component is higher than 40°. The change in the target morphology and the dependence of the composition of the ablated material on local fluence, along with the hydrodynamic effects, is sought to explain this previously unexpected and unreported phenomenon. PACS 61.80.Ba; 47.35.+i; 52.38.Mf; 81.15.Fg     

Metal thin film ablation with femtosecond pulsed laser

Micromachining thin metal films coated on glass are widely used to repair semiconductor masks and to fabricate optoelectrical and MEMS devices. The interaction of lasers and materials must be understood in order to achieve efficient micromachining. This work investigates the morphology of thin metal films after machining with femtosecond laser ablation using about 1 μm diameter laser beam. The effect of the film thickness on the results is analyzed by comparing experimental images with data obtained using a two-temperature heat transfer model. The experiment was conducted using a high numerical aperture objective lens and a temporal pulse width of 220 fs on 200- and 500-nm-thick chromium films. The resulting surface morphology after machining was due to the thermal incubation effect, low thermal diffusivity of the glass substrate, and thermodynamic flow of the metal induced by volumetric evaporation. A Fraunhofer diffraction pattern was found in the 500-nm-thick film, and a ripple parallel to the direction of the laser light was observed after a few multiple laser shots. These results are useful for applications requiring micro- or nano-sized machining.     

激光烧蚀金属Al诱导发光的动力学研究

利用时间分辨的光谱测量技术,测定了XeCl紫外激光在不同条件下烧蚀金属Al诱导产生光谱线及其强度随时间的分布.结果表明：等离子体辐射光谱线由原子光谱线、一价离子光谱线及连续辐射背景光组成.Al原子光谱线的辐射强度与持续时间为最大,一价离子光谱线次之,以连续辐射背景光为最小.对激光烧蚀金属诱导发光的机理进行了探讨.等离子体中连续辐射背景光来自高能电子的韧致辐射和电子与离子的复合,原子光谱线和一价离子光谱线主要来自等离子体中电子与离子的复合.用此机理定性地解释了所观察到的实验现象. 关键词： 激光烧蚀 时间分辨光谱 辐射机理 金属Al     

Non-equilibrium plasma production by pulsed laser ablation of gold

A gold target has been irradiated with a Q-switched Nd:Yag laser having 1064?nm wavelength, 9?ns pulse width, 900?mJ maximum pulse energy and a maximum power density of the order of 10¹⁰?W/cm². The laser–target interaction produces a strong gold etching with production of a plasma in front of the target. The plasma contains neutrals and ions having a high charge state. Time-of-flight (TOF) measurements are presented for the analysis of the ion production and ion velocity. A cylindrical electrostatic deflection ion analyzer permits measurement of the yield of the emitted ions, their charge state and their ion energy distribution. Measurements indicate that the ion charge state reaches 6⁺ and 10⁺ at a laser fluence of 100?J/cm² and 160?J/cm², respectively. The maximum ion energy reaches about 2?keV and 8?keV at these low and high laser fluences, respectively. Experimental ion energy distributions are given as a function of the ion charge state. Obtained results indicate that electrical fields, produced in the plume, along the normal to the plane of the target surface, exist in the unstable plasma. The electrical fields induce ion acceleration away from the target with a final velocity dependent on the ion charge state. The ion velocity distributions follow a “shifted Maxwellian distribution”, which the authors have corrected for the Coulomb interactions occurring inside the plasma.