Double-pulse LIBS of gadolinium oxide ablated by femto- and nano-second laser pulses

Emission characteristics of gadolinium (Gd) oxide are studied, using ns and fs laser pulses for ablation in double-pulse laser induced breakdown spectroscopy (LIBS). In the current conditions of pulse energy and signal detection timing, emission intensity enhancement in the reheating mode is 25-fold, but little effect can be observed in a pre-pulse mode. It is shown that the optimum focus position of the ablation pulse is about 5 mm apart from the sample surface in the reheating mode. Although little emission can be observed in the single-pulse configuration with fs ablation pulses, the intense emission can be observed in the reheating mode in the double-pulse configuration.     

固体壁面附近激光空泡的动力学特性研究

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Simulation of ultrashort double-pulse laser ablation

In this paper, we study the mechanisms of femtosecond double-pulse laser ablation of metals. It was previously shown experimentally that the crater depth monotonically drops when the delay between two successive pulses increases. For delays longer than the time of electron-ion relaxation the crater depth can be even smaller than that produced by a single pulse. The results of the performed hydrodynamic simulation show that the ablation can be suppressed due to the formation of the second shock wave. The modeling results of the double-pulse ablation obtained for different delays correlate with the experimental findings.     

偏振态对飞秒激光加工石英玻璃表面质量的影响

为研究线偏振和圆偏振对飞秒激光烧蚀加工石英玻璃表面质量的影响,开展不同扫描速度的线烧蚀试验和不同线重叠率的面烧蚀试验。研究了线、圆偏振光对烧蚀线宽度的影响,利用光学显微镜和环境扫描电子显微镜观察烧蚀形貌,并使用三维表面轮廓仪进行烧蚀面粗糙度分析。结果表明:线偏振光烧蚀线宽度大于圆偏振光,且激光功率越大,线宽差异越明显;当线重叠率在65%~90%时,线偏振光烧蚀表面粗糙度随重叠率增大而增大,在重叠率为65%时达到1.33μm;线轮廓算术平均偏差随重叠率增大先减小后增大,并在重叠率为80%时达到较小值1.05μm;当重叠率不到80%时,线偏振光烧蚀面线轮廓算术平均偏差比圆偏振光小;重叠率为90%时,其线轮廓算术平均偏差反而比圆偏振光大。     

激光烧蚀高纯Zn形成的微米金属球体对后续脉冲激光的耦合增强效应

脉冲激光束在低真空(约2 Pa)环境下聚焦到高纯Zn靶表面, 烧蚀区域不仅有中心深孔的宏观损伤, 而且还发现大量微米量级的类似足球形状的金属Zn球体结构附着生长在孔洞内侧表面. 实验过程中采用等离子体光谱诊断技术研究宏观和微观损伤对后续脉冲激光的影响程度. 与聚焦于金属Zn平滑表面相比, 宏观损伤可以使后续激光诱导的Zn原子334.5 nm谱线强度提高10.3%, 在此基础上大量Zn微米球体附着在内表面可以使谱线强度再提高34.3%. 因此, 推断这些金属Zn微球表面镶嵌着光洁的纳米量级六边形和五边形小平面, 可以对后续脉冲激光产生镜面反射, 使得激光能量汇聚并耦合增强, 提高烧蚀效率. 实验结果还表明, 这些微米球体的数目随着激光脉冲次数的增加而增多, 使得后续激光能够诱导产生更为致密高温的等离子体. 研究结果有望为激光-金属微孔技术提供新思路. 关键词： 脉冲激光烧蚀 微纳米结构 激光诱导等离子体     

Plasma property effects on spectral line broadening in double-pulse laser-induced breakdown spectroscopy

Double-pulse Laser-Induced Breakdown Spectroscopy (LIBS) in an orthogonal configuration was used to investigate plasma temperature and electron density effects on Mg II emission spectral line broadening. The experiments were carried out with two Nd:YAG lasers, one operating at 355 nm for ablation and the other one at 1064 nm for plasma reheating in air at atmospheric pressure. Temporally resolved plasma temperature and electron density were measured at various delay times. Data in this study show prolonged emission of Mg II (280.27 nm) as well as enhancement of the signal intensity when using double-pulse excitation compared to the single-pulse case. An enhancement of ～8× was attained with a delay between the laser pulses equal to 1 μs. The enhancement was accompanied by higher plasma temperature and increased electron density. The double-pulse LIBS configuration provides energy to sustain the plasma emission at a period in time when the linewidth is minimum, thereby improving the analytical capabilities of low spectral resolution instrumentation typically used in LIBS system.     

Impact of an extended source in laser ablation using pulsed digital holographic interferometry and modelling

Pulsed digital holographic interferometry has been used to study the effect of the laser spot diameter on the shock wave generated in the ablation process of an Nd:YAG laser pulse on a Zn target under atmospheric pressure. For different laser spot diameters and time delays, the propagation of the expanding vapour and of the shock wave were recorded by intensity maps calculated using the recorded digital holograms. From the latter, the phase maps, the refractive index and the density field can be derived. A model was developed that approaches the density distribution, in particular the ellipsoidal expansion characteristics. The induced shock wave has an ellipsoid shape that approaches a sphere for decreasing spot diameter. The ellipsoidal shock waves have almost the same centre offset towards the laser beam and the same aspect ratio for different time steps. The model facilitates the derivation of the particle velocity field. The method provides valuable quantitative results that are discussed, in particular in comparison with the simpler point source explosion theory.     

Laser ablation of powdered samples and analysis by means of laser-induced breakdown spectroscopy

The presented work proves the capacities of laser-induced breakdown spectroscopy (LIBS) as a fast, universal, and versatile technique for analysis of complex materials as ceramics. This paper reports on the analysis of ceramic raw materials (brick clays and kaolin) submitted to laser ablation in the form of pressed pellets. Spectrographic study was provided by standard single-pulse LIBS technique and orthogonal reheating double-pulse LIBS. It was found that both methods are comparable in terms of analytical performance, if adequate experimental parameters and signal detection systems are used.     

Double-pulse neodymium YAG/Carbon dioxide laser-induced breakdown spectroscopy for excitation of bulk and trace analytes

The mechanisms involved in signal enhancement and persistence of the plasma in double-pulse laser-induced breakdown spectroscopy are investigated, and their implications to improving figures of merit for bulk and trace analytes in sample are discussed. For double-pulse laser-induced breakdown spectroscopy, 1064 nm neodymium YAG laser is used for ablation and 10.6 µm transversely excited atmospheric carbon dioxide laser in near-collinear geometry is used for reheating. Significant improvement in signal detection and sensitivity of both bulk and trace analytes using double-pulse laser-induced breakdown spectroscopy as compared to conventional single-pulse laser-induced breakdown spectroscopy are observed. Using double-pulse laser-induced breakdown spectroscopy in near-collinear geometry, Cu and Fe as bulk and trace analytes, respectively, in brass sample, showed 5 and 6 times improvement in persistence of the spectral emission. Temporal and time-integrated studies show that ionic lines are significantly enhanced compared to neutral lines. Plasma characterization employing spectroscopic methods showed significant enhancement in plasma temperature resulting in higher signal as well as increased plasma persistence of the species studied.     

超短激光蚀除金属机制的分子动力学研究

 采用耦合电子热传导方程的分子动力学方法,研究了飞秒激光辐照下金属Ni的熔化及蚀除动力学。分析了靶材内部温度分布特征及蚀除产物的构成,主要包含单个原子及大团簇。确定了断裂位置和蚀除开始的标志,即该处温度分布出现小的峰值,且粒子数密度急剧下降。模拟结果表明：强烈的蒸发及靶材内部所产生的拉应力分别是单个原子及大团簇喷射的机制。同时,深入探讨了激光诱导压力波的传播规律,预测了压力波的波速,约为4.97 km/s。将不同脉冲能量密度下的蚀除速率同实验数据加以对比,结果相差16%~20%。预测了熔深随时间的变化规律,基本随时间的延续而呈上升的趋势。发现过热现象的存在。     

Laser drilling of stainless steel with nanosecond double-pulse

Nanosecond double-pulse laser drilling is reported in this paper. The double-pulse herein represents two closely conjoint pulses with 21 ns pulse duration and about 52 ns interpulse separation, which are acquired by temporal pulse shaping. Percussion drilling with such double-pulse is performed in stainless steel samples with different laser fluences, sample's thickness, repetition rates and ambient pressures. The experimental results show that the drilling rates of double-pulse drilling are more than one order of magnitude higher than that of conventional single-pulse drilling in air. Differences in the processing results between single-pulse and double-pulse with various processing parameters are investigated. In addition the ablation mechanisms of the double-pulse drilling are discussed.     

Role of the wall ablation in the operation of a 46.9 nmAr capillary discharge soft x‐ray laser

A capillary discharge pumped soft x‐ray laser operating at 46.9 nm on the 3p–3s transition of the Ne‐like Ar has been realized by pumping the active medium with a relatively slow current pulse (dI/dt ≈ 6 · 10¹¹ A/s). In order to study the role of the ablation in the production of the laser effect, the intensity of the amplified 46.9 nm line has been investigated using the same pumping current pulses in the plastic (polyacetal) and ceramic (Al₂O₃). We showed that the ablation of the capillary walls is unfavorable both for the compression and stability of the plasma and consequently for the soft x‐ray laser production. The amplification and lasing effects are observed only in the ceramic channel. The measurements of the line intensity at 46.9 nm showed the lasing with a gain‐length product of ≈ 9, a laser pulse energy of ≈ 5 μJ, a pulse duration of 1.3 ns and a beam divergence of ≈ 3.5 mrad. In addition, effect of the scaling of the time of lasing with the initial plasma diameter was demonstrated experimentally and compared with a one‐dimensional MHD model.     

外加静电场下激光诱导等离子体电子、离子特性的实验研究

从局部热平衡等离子体的一价铝离子速度服从麦克斯韦-玻尔兹曼分布出发,导出了电流信号的时间演化函数,通过对实验曲线拟合,得到激光诱导铝等离子体中一价铝离子的平动温度.实验研究了电流信号强度与外加电压之间的关系.实验结果说明电流信号强度随外加电压的增加而增大但并非线性增长而且与缓冲气体的性质和靶样品的物理特性有关.     

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.     

Silicon micro-hemispheres with periodic nanoscale rings produced by the laser ablation of single crystalline silicon

We describe the fabrication of silicon micro-hemispheres by adopting the conventional laser ablation of single crystalline silicon in the vacuum condition without using any catalysts or additives. The highly oriented structures of silicon micro-hemispheres exhibit many periodic nanoscale rings along their outer surfaces. We consider that the self-organized growth of silicon micro-structures is highly dependent on the laser intensity and background air medium. The difference between these surface modifications is attributed to the amount of laser energy deposited in the silicon material and the consequent cooling velocity.     

纳秒脉冲激光沉积薄膜过程中的烧蚀特性研究

研究了高能短脉冲激光薄膜制备的整个烧蚀过程.首先建立了基于超热理论的烧蚀模型，然 后利用较为符合实际的高斯分布表示脉冲激光输入能量密度，给出了考虑蒸发效应不同阶段 的烧蚀状态方程.结合适当的边界条件，以Si靶材为例，利用有限差分法得到了靶材在各个 阶段温度随时间和烧蚀深度的演化分布规律及表面蒸发速度与烧蚀深度在不同激光辐照强度 下随时间的演化规律.结果表明，在脉冲激光辐照阶段，靶材表面的蒸发效应使得靶材表面 温度上升显著放缓；在激光辐照强度接近相爆炸能量阈值时，蒸发速度与蒸发厚度的变化由 于逆流现象将显著放缓.还得到了考虑了熔融弛豫时间及蒸发效应的固-液界面随时间的演化 方程，这一结论较先前工作更具有普适性. 关键词： 脉冲激光烧蚀 热流方程 温度演化 有限差分法     

Energy distribution of ions in plasma formed by laser ablation of metallic Nb and Ta targets

The laser plasma plume expansion induced by UV nanosecond irradiation from metallic Nb and Ta targets has been studied using Langmuir probe time-of-flight measurements. The ion current shape was measured as a function of the laser radiation flux at various probe-to-target distances. The ion velocity distribution and the ion energy spectra have been determined by measuring the time of flight of ions reaching the Langmuir probe. A multi-mode velocity distribution of ions has been revealed. The dependence of the amplitudes of the plume energy components on the plume scatter time and on the laser radiation flux has been investigated. The experimental time-of-flight data have been compared with a Maxwell velocity distribution. The threshold values of the laser intensity were determined for different distribution modes in the ion energy spectrum.     

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.     

Dynamics of femtosecond laser-produced plasma ions

We investigated the ion laser-produced plasma plume generated during ultrafast laser ablation of copper and silicon targets in high vacuum. The ablation plasma was induced by ≈50 fs, 800 nm Ti:Sa laser pulses irradiating the target surface at an angle of 45°. An ion probe was used to investigate the time-of-flight profiles of the emitted ions in a laser fluence range from the ablation threshold up to ≈10 J/cm². The angular distribution of the ion flux and average velocity of the produced ions were studied by moving the ion probe on a circle around the ablation spot. The angular distribution of the ion flux is well described by an adiabatic and isentropic model of expansion of a plume produced by laser ablation of solid targets. The angular distribution of the ion flux narrows as the laser pulse fluence increases. Moreover, the ion average velocity reaches values of several tens of km/s, evidencing the presence of ions with kinetic energy of several hundred eV. Finally, the ion flux energy is confined in a narrow angular region around the target normal.     

Pulsed laser ablation of borocarbide targets probed by time-of-flight mass spectrometry

Excimer laser ablation of superconductive borocarbide material (YNi₂B₂C) in typical conditions for the deposition of superconductive thin films has been investigated using time-of-flight mass spectrometry. The mass spectra show the presence of all the target elemental ionized atoms as well as diatomics. The ablation yield of the metal ions is a strongly increasing function of the laser fluence, while the contrary is true for non-metal ions. The dependence of non-metal light mass diatomic ions on laser fluence indicates the presence of aggregation processes as the laser fluence is increased. Moreover, evidence of aggregation processes involving metallic ions at high laser fluence is also obtained by the mass spectra. An interesting aspect of our results is the observation of an ion spatial distribution characterized by the presence of the lighter species at the plume edges, while the heavier ones are concentrated at the plume center.