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.     

Time-resolved PLIF imaging of Cu in a laser-ablated copper plasmaplume

Planar laser-induced fluorescence (PLIF) has been used to determine the relative number density of ground state copper atoms in laser-ablated plasma plumes. An ablation laser power flux of ~1.5 GW/cm ² is applied to a solid copper target in a background gas, producing a plasma plume suitable for studying homogeneous copper vapor condensation. Density is measured at postablation time delays ranging from 5 μs to 10 ms with 1-100 torr of either argon or helium as the background gas. Planar laser-induced fluorescence images are used to spatially resolve the relative density within the plume, The decrease in density is due to the homogeneous condensation of copper vapor to form particulate     

超短脉冲激光烧蚀石墨产生的喷射物的时间分辨发射光谱研究

本文使用不同激光能流(18 J/cm²–115 J/cm²)和脉冲宽度(50 fs–4 ps)的超短脉冲激光在真空中(4×10^-4 Pa)烧蚀高定向热解石墨. 通过测量烧蚀喷射物的时间分辨发射光谱研究喷射物的超快时间演化. 在喷射物发射光谱中, 观察到了C₂基团的天鹅带光谱系统, 416 nm附近C₁₅基团的由电子能级¹Σ_u⁺ 和¹Σ_g⁺之间的振动跃迁产生的光谱峰以及连续谱. 50 fs, 115 J/cm²的脉冲激光烧蚀产生的喷射物的连续谱的强度衰减分为快速下降和慢速下降两个阶段(以20 ns时间延迟为分界). 这表明连续谱是由两种不同的组分贡献的. 快速下降阶段, 连续谱主要由碳等离子体通过韧致辐射产生; 慢速下降阶段, 连续谱主要由烧蚀后期产生的大颗粒碳簇的热辐射贡献. 实验结果还揭示了激光能流的提高, 会明显增加喷射物中碳等离子体和激发态C₂的含量, 但对质量稍大的C₁₅的影响较小; 此外, 50 fs脉冲激光烧蚀产生的连续谱的存在时间会随着激光能流的减小而增大, 这说明低能流更有利于在烧蚀后期产生碳簇. 脉宽主要影响喷射物连续谱的时间演化. 4 ps脉冲激光烧蚀产生的连续谱的整个时间演化过程明显慢于50 fs脉冲产生的连续谱.     

Optical transmission and reflection of aluminum film irradiated by nanosecond laser beam and experimental studying of phase-explosion

In this paper we present evidence for a phase explosion during the laser-induced ablation process by studying the optical reflectivity of the ablated plume. The ablation was produced by irradiating thin film aluminum coated on a quartz substrate with a single pulse laser beam in ambient air. The laser pulse was provided by the second harmonic of a Q-switched Nd:YAG laser with ∼10 ns pulse duration. The transmission of a low power He–Ne laser beam through the hot ablated material plume and its reflection (from the front surface, and rear surface of aluminum film) were also monitored during the duration of the ablation event. The results show that the front surface reflectivity is enhanced at an early time of ablation which is described as strong evidence for the creation of a phase explosion in this process.     

Temporal evolution of laser-ablated Co ions probed by time-of-flight mass spectrometry

A pulsed-field time-of-flight mass spectrometric (TOFMS) technique was used to investigate the expansion dynamics of the ionic species ejected from the visible (λ=532 nm) laser ablation of cobalt target at low laser fluence less than 1 J/cm². The temporal evolution of Co⁺ ions was studied by varying the delay time of the ion repelling pulse with respect to the laser irradiation, which provides significant information on the ablated plume characterization. The obtained TOF mass spectra were well fitted by shifted Maxwell–Boltzmann distributions on a stream velocity, commonly used to describe the measured velocity distributions. The TOF distribution of Co⁺ ions showed a bimodal distribution with fast and slow velocities. These velocities show a decreasing tendency with delay time, which is attributed to the gas collisions between the plume ejecta and to the related gas dynamics. The present results suggest that the in situ measurements of the most probable velocity of ablated ions along the normal to the solid target can be accomplished by the simple technique of a laser ablation/TOFMS.     

激光烧蚀金属表面产生的发射光谱分析

用观测时间和空间分辨发射光谱的方法研究了脉冲激光烧蚀金属铝靶过程中产生的等离子体羽的特性，计算了其膨胀速度，讨论了大气中等离子体点燃的机制。     

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.     

Expansion dynamics of the plasma plume created by laser ablation in a background gas

The dynamics of the expansion of the plasma plume induced by laser ablation of a copper target at a fluence of 17 J/cm² was investigated theoretically by means of a Monte Carlo simulation. When the expansion occurs under a relatively high pressure, the ambient gas particles may be involved in the collective motion of the plume. The simulation allows the study of the simultaneous collective motion of different species, such as the laser-ablated and the ambient gas particles. The influence of the background gas nature and pressure on the laser-induced plasma plume expansion behavior was studied. The expansion dynamics were found to be different in the case of the expansion in ambient gases of different molecular weight. The dynamics of the plume expansion under an argon pressure of 200 Pa seem to be strongly related to the equilibration of the pressure gradients in the gas phase, and evidence of the oscillatory behavior of the plume expansion was shown from the evolution over time of the pressure profiles in the plume. This behavior has also been observed in similar conditions for a krypton atmosphere, but for a lower pressure than for argon. The vortical flow formation at the plume periphery, involving both the laser-ablated and the argon particles at moderate pressure, was also predicted from the Monte Carlo simulation.     

Formation process of Si nanoparticles in rare gas observed by a decomposition method

We have investigated the formation process of silicon nanoparticles after laser ablation of silicon targets in argon gas. The nanoparticles exhibit bright photoluminescence in the visible wavelength range and can be applied to opto-electronic devices. In order to observe silicon nanoparticles, we have developed a decomposition method. The nanoparticles were probed by detecting light emission resulting from decomposition using a second laser. This method enables us to observe nanoparticles that cannot be observed directly by the methods applied so far. We have observed that the nanoparticles grow in time periods of 1.0-1.8 ms following ablation in Ar gas at 5 Torr when Si targets are ablated at 5 J/cm² with a pulse width of 7 ns. The nanoparticles begin to grow above ablation spots slightly apart from the targets just after thermalization of the plume. We also found that the growth is delayed at higher fluxes of ablation laser light.     

Measurement of laser beam transmittance through laser produced vapour plume

Laser produced plume, consisting of vapor front and ejected substrate on the workpiece surface, is an intermediate between the incident laser beam and the workpiece on which the beam is directed. It partially blocks, defocuses, absorbs, scatters, and deflects the incident beam and thereby reduces the laser energy reaching the workpiece. However, plume additionally acts as a heat source enhancing the machining. Consequently, laser induced plume plays an important role in laser machining process. The present study investigates the transmittance of a reference beam by the plume generated during the laser-workpiece interaction. To achieve the transmittance measurements, a Nd:YAG laser was used and four different materials were employed in the experiment. To obtain realistic values of the plume transmittance in relation to the laser machining process, the reference beam was sampled from the incident laser beam. The study was extended to include the effect of the laser pulse parameters on the transmission process. It is found that about 10–30% of the transmittance of the reference beam through a vapor plume, produced due to laser ablation, occurs close to the workpiece surface.     

Time-resolved dynamics analysis of nanoparticles applying dual femtosecond laser pulses

The evolution of a fs laser generated plume on copper was studied by dual laser pulses. The plume generated by the first pulse (620 nm) was excited by the second, delayed pulse (310 nm). The actual state of the plume was monitored by detecting the intensities of the emitted light and the reflected delayed pulse from the interaction range, i.e. 0–150 μm above the surface. Four peaks were observed in the 0–1400 ps time range and assigned to appearance of electrons, ions, atomic species and nanoparticles. Accordingly, the timing of the creation and ejection of these species was determined. By integrating the intensity of the nanoparticle peak, the production yield of the nanoparticles and its dependence on the ablating laser fluence was calculated. The ablation products were deposited on a Si substrate, too, and analyzed by atomic force microscopy and scanning electron microscopy. The results of the deposition and the dual-pulse experiments are in good agreement with the theory. PACS 52.38.Mf; 79.20.Ds; 61.80.Ba     

Non-contact acoustic tests based on nanosecond laser ablation: Generation of a pulse sound source with a small amplitude

A method to generate a pulse sound source for acoustic tests based on nanosecond laser ablation with a plasma plume is discussed. Irradiating a solid surface with a laser beam expands a high-temperature plasma plume composed of free electrons, ionized atoms, etc. at a high velocity throughout ambient air. The shockwave generated by the plasma plume becomes the pulse sound source. A laser ablation sound source has two features. Because laser ablation is induced when the laser fluence reaches 10¹²–10¹⁴ W/m², which is less than that for laser-induced breakdown (10¹⁵ W/m²), laser ablation can generate a lower sound pressure, and the sound source has a hemispherical radiation pattern on the surface where laser ablation is generated. Additionally, another feature is that laser-induced breakdown sound sources can fluctuate, whereas laser ablation sound sources do not because laser ablation is produced at a laser beam–irradiation point. We validate this laser ablation method for acoustic tests by comparing the measured and theoretical resonant frequencies of an impedance tube.     

Nonstationary heating during VUV photochemical ablation of polymers

According to a previously developed pure photochemical model of VUV laser ablation of polymers, the velocity of ablation front is proportional to surface intensity, and a stationary value of the surface temperature does not depend on laser intensity. Previous estimations show, however, that this stationary surface temperature could be too high to be relevant to the photochemical mechanism. This raises a question of whether the stationary value of the surface temperature can be achieved for a given time shape of light intensity coming to the surface irradiated by a laser pulse of high enough fluence. The intensity time shape is connected not only with the time shape of a laser pulse but also with screening of laser radiation by the plume. This problem is discussed in the present communication. Specifically, it is shown that with a hyperbolic surface intensity time shape, heat diffusion can successfully compete with laser heating decreasing maximum surface temperature compared to its stationary value. The hyperbolic surface laser intensity corresponds to a rectangular laser pulse screened by plume during the photochemical ablation. This allows one to estimate that the photochemical model for a multiple-pulse VUV laser ablation with a high plume extinction coefficient is self-consistent even for a high value of stationary temperature and for high enough laser fluences. PACS 42.62.-b; 44.05.+e; 82.53.-k     

Features of plasma plume evolution and material removal efficiency during femtosecond laser ablation of nickel in high vacuum

We present an experimental characterization describing the characteristics features of the plasma plume dynamics and material removal efficiency during ultrashort, visible (527 nm, ≈300 fs) laser ablation of nickel in high vacuum. The spatio-temporal structure and expansion dynamics of the laser ablation plasma plume are investigated by using both time-gated fast imaging and optical emission spectroscopy. The spatio-temporal evolution of the ablation plume exhibits a layered structure which changes with the laser pulse fluence F. At low laser fluences (F<0.5 J/cm²) the plume consists of two main populations: fast Ni atoms and slower Ni nanoparticles, with average velocities of ≈10⁴ m/s for the atomic state and ≈10² m/s for the condensed state. At larger fluences (F>0.5 J/cm²), a third component of much faster atoms is observed to precede the main atomic plume component. These atoms can be ascribed to the recombination of faster ions with electrons in the early stages of the plume evolution. A particularly interesting feature of our analysis is that the study of the ablation efficiency as a function of the laser fluence indicates the existence of an optimal fluence range (a maximum) for nanoparticles generation, and an increase of atomization at larger fluences. PACS 52.50.-b; 52.38.Mf; 79.20.Ds; 81.07.-b     

Analysis of the sizes and number of microparticles in the ablation plume,which attenuates laser radiation during ablation of a constructive material

The effect of laser radiation with a wavelength of 1.3 μm, power of 25 kW, pulse width of 1 s, and irradiated spot area of 9 cm² on carbon silicon carbide composite material (CSCCM) is analyzed. The formation of an ablation plume (which consists of vapor of irradiated material, burning products, drops and microparticles of various chemical composition and size) above the irradiated surface leads to a significant loss of laser energy. The fractions of the scattered and absorbed laser radiation in the plume are determined, the size and mass distributions of microparticles in the plume are estimated, their concentration is calculated, and the microparticle escape velocities from the irradiated CSCCM surface are evaluated.     

Measurement of Er:YAG laser ablation plume dynamics

The dynamics of tissue ablation using an Er:YAG laser were studied using flash photography and optical pump-probe techniques. Both normal-spiking-mode and Q-switched Er:YAG laser radiation were used to study the ablation of skin and bone. Time-resolved photographs of the ablation plume were obtained using a microscope-mounted camera together with pulsed illumination from an excimer-pumped dye laser. The velocity of the plume front, obtained from the photographs, was approximately 1400 m/s. The same velocity was also measured using an optical pump-probe technique. Both techniques indicate that material removal occurred after the end of the 90-ns-long Q-switched laser pulse and that each micropulse in the normal-spiking-mode pulse train was capable of ablating and rapidly ejecting tissue.This work was supported in part by the SDIO-MFEL Program under contract # N00014-86-K-0117 and by the Arthur O. and Gullan M. Wellman Foundation     

Molecular dynamics simulations of cluster distribution from femtosecond laser ablation in aluminum

Femtosecond laser ablation and plume evolution of aluminum is investigated for various inhomogeneous laser pulses. For the simulations of the atoms the molecular dynamics code IMD is used. The ablated gas-phase is scanned by a cluster algorithm (DBSCAN), from which we gain a cluster size distribution of the ablated material. Per single pulse, only a small portion of the total volume evaporates into the gas phase. Therefore??to have reasonable statistics??we have to deal with huge samples (6×10⁷?atoms). The ablation threshold is determined by comparing the depth of the holes to the applied fluence. Angular and velocity distributions of the plume are compared to experiments.     

Comparison of the laser ablation process on Zn and Ti using pulsed digital holographic interferometry

Pulsed digital holographic interferometry has been used to compare the laser ablation process of a Q-switched Nd-YAG laser pulse (wavelength 1064 nm, pulse duration 12 ns) on two different metals (Zn and Ti) under atmospheric air pressure. Digital holograms were recorded for different time delays using collimated laser light (532 nm) passed through the volume along the target. Numerical data of the integrated refractive index field were calculated and presented as phase maps. Intensity maps were calculated from the recorded digital holograms and are used to calculate the attenuation of the probing laser beam by the ablated plume. The different structures of the plume, namely streaks normal to the surface for Zn in contrast to absorbing regions for Ti, indicates that different mechanisms of laser ablation could happen for different metals for the same laser settings and surrounding gas. At a laser fluence of 5 J/cm², phase explosion appears to be the ablation mechanism in case of Zn, while for Ti normal vaporization seems to be the dominant mechanism.     

纳秒激光烧蚀冲量耦合数值模拟

为研究激光烧蚀靶产生冲量过程和机理, 建立了一个复杂的一维热传导和流体动力学模型. 以空间碎片常见材料Al为例, 用建立的模型数值计算了纳秒脉宽激光烧蚀靶产生的冲量及冲量耦合系数随时间变化情况. 数值结果和已有的实验数据符合的较好. 数值计算表明: 激光脉冲时间内, 靶获得的冲量随时间迅速增加, 在脉冲时间结束后, 冲量变化随时间趋于稳定; 在冲量耦合过程中, 烧蚀等离子体向真空膨胀, 羽流尺度逐渐增大, 同时吸收入射激光能量, 导致激光与靶耦合的能量降低. 关键词： 激光烧蚀 冲量耦合 等离子体     

Nanosecond and femtosecond ablation of La0.6Ca0.4CoO3: a comparison between plume dynamics and composition of the films

Thin films of La_0.6Ca_0.4CoO₃ were grown by pulsed laser ablation with nanosecond and femtosecond pulses. The films deposited with femtosecond pulses (248 nm, 500 fs pulse duration) exhibit a higher surface roughness and deficiency in the cobalt content compared to the films deposited with nanosecond pulses (248 nm, 20 ns pulse duration). The origin of these pronounced differences between the films grown by ns and fs ablation has been studied in detail by time-resolved optical emission spectroscopy and imaging. The plumes generated by nanosecond and femtosecond ablation were analyzed in vacuum and in a background pressure of 60 Pa of oxygen. The ns-induced plume in vacuum exhibits a spherical shape, while for femtosecond ablation the plume is more elongated along the expansion direction, but with similar velocities for ns and fs laser ablation. In the case of ablation in the background gas similar velocities of the plume species are observed for fs and ns laser ablation. The different film compositions are therefore not related to different kinetic energies and different distributions of various species in the plasma plume which has been identified as the origin of the deficiency of species for other materials.