Finite element simulation of pulsed laser ablation of titanium carbide

In the present paper, a 2D finite element model based on the heat-conduction equation and on the Hertz-Knudsen equation for vaporization was developed and used to simulate the ablation of TiC by Nd:YAG and KrF pulsed laser radiation. The calculations were performed for fluences of 8 and 10 J/cm², which according to experimental results obtained previously, correspond to large increases of the ablation rate. The calculated maximum surface temperature of the target for both lasers is higher than the estimated value of TiC critical temperature, corroborating the hypothesis that the increase of the ablation rate is explained by the explosive boiling mechanism.     

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.     

蒸气压对激光辐照靶材烧蚀速率的影响

研究了强激光辐照碳/碳复合材料靶材引起的烧蚀现象及蒸气压对烧蚀速率的影响。基于傅里叶定律,建立了强激光辐照靶材的热传导模型,模拟了忽略蒸气压影响时烧蚀速率随功率的变化;通过Mott-smith近似方法描述了Knudsen层间断区域,分析了间断两侧表面粒子状态参数;结合质量连续方程和蒸气压与温度关系方程,并由气体状态方程描述蒸气流状态,对蒸气压条件下激光烧蚀碳/碳复合材料靶材的速率随功率变化的关系进行了数值模拟。结果表明,在高能激光对靶材的烧蚀过程中,蒸气压力变化会导致靶材的饱和蒸气温度发生变化,进而影响烧蚀速率且使其随功率呈非线性变化,与忽略蒸气压作用时的线性变化规律相差较大,从理论上解释了忽略蒸气压导致的实验数据与理论结果的差异。     

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.     

Pulsed laser evaporation: equation-of-state effects

Theoretical study of laser ablation is usually based on the assumption that the vapor is an ideal gas. Its flow is described by gas dynamics equations [1, 2]. The boundary conditions at vaporization front are derived from the solution of the Boltzmann equation that describes the vapor flow in the immediate vicinity of the vaporizing surface (so-called Knudsen layer) [1]. This model is applicable within the range of temperatures much lower than the critical temperature of target material. In the present work, a general case is considered when the temperature of the condensed phase is comparable to or higher than the critical temperature. The dynamics of both condensed and gaseous phases can be described in this case by the equations of hydrodynamics. The dynamics of vaporization of a metal heated by an ultrashort laser pulse is studied both analytically and numerically. The analysis reveals that the flow consists of two domains: thin liquid shell moving with constant velocity, and thick low-density layer of material in two-phase state. Received: 2 March 1999 / Accepted: 28 May 1999 / Published online: 21 October 1999     

Mechanisms of Resonant Infrared Matrix-Assisted Pulsed Laser Evaporation

For the last decade, a variant of pulsed laser ablation, Resonant-Infrared Matrix-Assisted Pulsed Laser Evaporation (RIR-MAPLE), has been studied as a deposition technique for organic and polymeric materials. RIR-MAPLE minimizes photochemical damage from direct interaction with the intense laser beam by encapsulating the polymer in a high infrared-absorption solvent matrix. This review critically examines the thermally-induced ablation mechanisms resulting from irradiation of cryogenic solvent matrices by a tunable free electron laser (FEL). A semi-empirical model is used to calculate temperatures as a function of time in the focal volume and determine heating rates for different resonant modes in two model solvents, based on the thermodynamics and kinetics of the phase transitions induced in the solvent matrices. Three principal ablation mechanisms are discussed, namely normal vaporization at the surface, normal boiling, and phase explosion. Normal vaporization is a highly inefficient polymer deposition mechanism as it relies on collective collisions with evaporating solvent molecules. Diffusion length calculations for heterogeneously nucleated vapor bubbles show that normal boiling is kinetically limited. During high-power pulsed-FEL irradiation, phase explosion is shown to be the most significant contribution to polymer deposition in RIR-MAPLE. Phase explosion occurs when the target is rapidly heated (10⁸ to 10¹⁰ K/s) and the solvent matrix approaches its critical temperature. Spontaneous density stratification (spinodal decay) within the condensed metastable phase leads to rapid homogeneous nucleation of vapor bubbles. As these vapor bubbles interconnect, large pressures build up within the condensed phase, leading to target explosions and recoil-induced ejections of polymer to a near substrate. Phase explosion is a temperature (fluence) threshold-limited process, while surface evaporation can occur even at very low fluences.     

Vaporization and Plasma Shielding during High Power Nanosecond Laser Ablation of Silicon and Nickel

A thermal model to describe the high-power nanosecond pulsed laser ablation is presented. It involves the vaporization and the following plasma shielding effect on the whole ablation process. As an example of Si target, we obtainthe time evolution of the calculated surface temperature, ablation rate and ablation depth. It can be seen that plasma shielding plays a more important role in the ablation process with time. At the same time, the ablation depth with laser fluence based on different models is shown. Moreover, we simulate the pulsed laser irradiation Ni target. The evolution of the transmitted intensity and the variation of ablation depth per pulse with laser fluence are performed. Under the same experimental conditions, the numerical results calculated with our thermal model are more in agreement with the experimental data.     

热阻塞效应对激光辐照靶材烧蚀过程的影响分析

研究了百兆瓦级激光烧蚀碳/碳复合材料靶材产生的等离子体吸收激光束能量引起的热阻塞效应。首先,基于逆轫致吸收理论,建立了激光在烧蚀靶材产生的等离子体中的传播模型;然后,基于磁流体理论,得到了等离子体在百兆瓦级激光形成的电磁场中的波动方程,建立了等离子体吸收激光能量引起热阻塞效应的模型。最后,对烧蚀过程中粒子的总密度、吸收系数、靶材表面等效热流随激光持续时间的变化规律以及是否考虑热阻塞效应时,靶面垂直方向的温度场进行了数值模拟。结果表明:等离子体的形成,对激光形成了明显的热阻塞效应,削弱了激光对靶材的烧蚀作用,使粒子总密度、吸收系数、靶材表面等效热流以及靶面垂直方向温度场的变化均呈现为非线性。     

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.     

Pulsed laser ablation of solids: transition from normal vaporization to phase explosion

We present experimental data on mass removal during 1064-nm pulsed laser ablation of graphite, niobium and YBa₂Cu₃O_7-δ superconductor. Evidence for the transition from normal vaporization to phase explosion has been obtained for these materials, showing a dramatic increase in the ablation rate at the threshold fluences of 22, 15 and 17.5 J/cm², respectively. A numerical model is used to evaluate the ablation rate and temperature distribution within the targets under near-threshold ablation conditions. The results are analyzed from the viewpoint of the vaporized matter approaching the critical point with increasing laser fluence. A possible means of the estimating the thermodynamic critical temperature from the data for nanosecond laser ablation is discussed. It is suggested that the critical temperature of refractory metals is higher than that estimated with the traditional methods due to plasma effects. An analogy with the boiling crisis (the transition from nucleate to film boiling) is drawn to explain the formation of ablation craters with spallated edges. Received: 18 May 2000 / Accepted: 14 July 2000 / Published online: 22 November 2000     

XPS studies of short pulse laser interaction with copper

The effect of laser ablation on copper foil irradiated by a short 30 ns laser pulse was investigated by X-ray photoelectron spectroscopy. The laser fluence was varied from 8 to 16.5 J/cm² and the velocity of the laser beam from 10 to 100 mm/s. This range of laser fluence is characterized by a different intensity of laser ablation. The experiments were done in two kinds of ambient atmosphere: air and argon jet gas.The chemical state and composition of the irradiated copper surface were determined using the modified Auger parameter (α′) and O/Cu intensity ratio. The ablation atmosphere was found to influence the size and chemical state of the copper particles deposited from the vapor plume. During irradiation in air atmosphere the copper nanoparticles react with oxygen and water vapor from the air and are deposited in the form of a CuO and Cu(OH)₂ thin film. In argon atmosphere the processed copper surface is oxidized after exposure to air.     

Ultrafast solid–liquid–vapor phase change of a gold film induced by pico- to femtosecond lasers

Melting, vaporization and resolidification processes of thin gold film irradiated by a femtosecond pulse laser are studied numerically. The nonequilibrium heat transfer in electrons and lattice is described using a two-temperature model. The solid–liquid interfacial velocity, as well as elevated melting temperature and depressed solidification temperature, is obtained by considering the interfacial energy balance and nucleation dynamics. An iterative procedure based on energy balance and gas kinetics law to track the location of liquid–vapor interface is utilized to obtain the material removal by vaporization. The effect of surface heat loss by thermal radiation was discussed. The influences of laser fluence and duration on the evaporation process are studied. Results show that higher laser fluence and shorter laser pulse width lead to higher interfacial temperature, deeper melting and ablation depths.     

Laser ablation of a molten Ga target; comparison of experiments and simulation

The laser ablation mechanism of a molten Ga target was examined through comparison of experiments and simulation. The ablation was performed using an ArF excimer laser (193-nm wavelength and 20-ns duration) in vacuum. The observed existence of the threshold laser fluence (necessary for onset of the ablation) and linear increases in both the Ga deposition rate and the Ga emission (fluorescence) intensity with the laser fluence were satisfactorily explained by the simulation based on the thermal ablation model. In addition, it was found that most of the ablated particles are transferred to the substrate not in the form of an excited ion but an excited neutral atom, except at and near the target. Received: 3 September 2001 / Accepted: 7 November 2001 / Published online: 20 December 2001     

Phase transformation during surface ablation of cobalt-cemented tungsten carbide with pulsed UV laser

Surface ablation of cobalt-cemented tungsten carbide hard metal has been carried out in this work using a 308 nm, 20 ns XeCl excimer laser. Surface microphotography and XRD, as well as an electron probe have been used to investigate the transformation of phase and microstructure as a function of the pulse-number of laser shots at a laser fluence of 2.5 J/cm². The experimental results show that the microstructure of cemented tungsten carbide is transformed from the original polygonal grains of size 3 μm to interlaced large, long grains with an increase in the number of laser shots up to 300, and finally to gross grains of size 10 μm with clear grain boundaries after 700 shots of laser irradiation. The crystalline structure of the irradiated area is partly transformed from the original WC to βWC_1-x, then to αW₂C and CW₃, and finally to W crystal. It is suggested that the undulating ‘hill–valley’ morphology may be the result of selective removal of cobalt binder from the surface layer of the hard metal. The formation of non-stoichiometric tungsten carbide may result from the escape of elemental carbon due to accumulated heating of the surface by pulsed laser irradiation. Received: 13 July 2000 / Accepted: 27 October 2000 / Published online: 10 January 2001     

Thermal model for nanosecond laser sputtering at high fluences

The vaporization effect and the following plasma shielding generated by high-power nanosecond pulsed laser ablation are studied in detail based on the heat flux equation. As an example of Si target, we obtain the time evolution of the calculated surface temperature, ablation rate and ablation depth by solving the heat flow equations using a finite difference method. It can be seen that plasma shielding plays a more important role in the ablation process with time. At the same time, the variation of ablation depth per pulse with laser fluence is performed. Our numerical results are more agreed with the experiment datum than other simulated results. The result shows that the plasma shielding is very important.     

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.     

Thermoelastic wave induced by pulsed laser heating

In this work, a generalized solution for the thermoelastic plane wave in a semi-infinite solid induced by pulsed laser heating is developed. The solution takes into account the non-Fourier effect in heat conduction and the coupling effect between temperature and strain rate, which play significant roles in ultrashort pulsed laser heating. Based on this solution, calculations are conducted to study stress waves induced by nano-, pico-, and femtosecond laser pulses. It is found that with the same maximum surface temperature increase, a shorter pulsed laser induces a much stronger stress wave. The non-Fourier effect causes a higher surface temperature increase, but a weaker stress wave. Also, for the first time, it is found that a second stress wave is formed and propagates with the same speed as the thermal wave. The surface displacement accompanying thermal expansion shows a substantial time delay to the femtosecond laser pulse. On the contrary, surface displacement and heating occur simultaneously in nano- and picosecond laser heating. In femtosecond laser heating, results show that the coupling effect strongly attenuates the stress wave and extends the duration of the stress wave. This may explain the minimal damage in ultrashort laser materials processing. Received: 23 May 2000 / Accepted: 26 May 2000 / Published online: 20 September 2000     

Acoustic wave monitoring of the excimer laser ablation of YBCO high-Tc superconductor

Monitoring the amplitude and the delay of arrival of the pressure waves generated during the interaction of laser pulses with YBCO in air, we can determine the vaporization and the ablation thresholds, the etching rate, the change of the acoustic wave velocity and the effect of plasma shielding on the etching rate. The steep increase of the amplitude and the order-of-magnitude increase of the etching rate above the ablation threshold, suggest that the laser–target coupling mechanism changes from (thermal) vaporization below threshold to a rapid solid-to-gas phase transition. The dumping of the acoustic waves following the ablation with successive laser pulses correlates with the evolution of the YBCO high-T_c superconductor surface morphology, which is known to relate to the deposition rate and the surface morphology of pulsed-laser-deposited high-T_c thin films. Received: 7 January 2000 / Accepted: 9 October 2000 / Published online: 25 July 2001     

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     

Pulsed laser ablation of La0.5Sr0.5CoO3

The ablation process of La_0.5Sr_0.5CoO₃ by a spatial uniform 248 nm excimer laser beam has been characterized. Ablation rates, changes in the target surface morphology and composition have been studied as a function of the laser fluence. The dependence of the ablation rate on the laser fluence has been explained by a model based on plasma absorption. The threshold fluence for complete dissociation of the surface has been determined and is found equal to 0.7 J/cm². Above this threshold, a steady-state target surface condition is obtained within 30 pulses. Below the threshold fluence, CoO nuclei form, which have a pronounced effect on the target composition and morphology. In addition, ellipsometric and reflectance spectra have been measured in the photon energy range of 1.8 to 5.0 eV.