Ablation mechanism study on metallic materials with a 10 ps laser under high fluence

Single shot ablation of metallic materials of aluminium, titanium alloy (Ti6Al4V) and gold has been studied with 10 picoseconds (ps) laser pulses experimentally and theoretically. The ablation rate variation at high fluence was explained by a simplified predictive model based on critical-point phase separation (CPPS) theory. A comparison between experimental and numerical results inferred that CPPS may well be the dominant ablation mechanism for high fluence laser ablation at 10 ps laser duration.     

Transient reflectivity and transmission changes during plasma formation and ablation in fused silica induced by femtosecond laser pulses

We have studied the plasma formation and ablation dynamics in fused silica upon irradiation with a single 120 fs laser pulse at 800 nm by using fs-resolved pump-probe microscope. It allows recording images of the laser-excited surface at different time delays after the arrival of the pump pulse. This way, we can extract both the temporal evolution of the surface reflectivity and transmission, at 400 nm, for different spatial positions in the spots (and thus for different local fluences) from single series of images. At fluences well above the visible ablation threshold, a fast and large increase of the reflectivity is induced by the formation of a dense free-electron plasma. The maximum reflectivity value is reached within ≈1.5 ps, while the normalized transmission decreases within ≈400 fs. The subsequent temporal evolution of both transient reflectivity and transmission are consistent with the occurrence of surface ablation. In addition, the time-resolved images reveal the existence of a free-electron plasma distribution surrounding the visible ablation crater and thus formed at local fluences below the ablation threshold. The lifetime of this sub-ablation plasma is ≈50 ps, and its maximum electron density amounts to 5.5×10²² cm⁻³.     

High power single-shot laser ablation of silicon with nanosecond 355 nm

We report on high intensity single-shot laser ablation of monocrystalline silicon with a nanosecond Nd:YAG at 355 nm. It is shown that for incident laser intensities exceeding ∼11.5 GW/cm² on the silicon surface, unusually high etch depths can be achieved reaching values up to 60 μm. The results support previous observations of dramatic increase in etch rates in single-shot laser ablation at 266 nm. A laser-induced explosive boiling mechanism together with secondary plasma heating is believed to be associated with this effect.     

355 nm皮秒激光辐照下熔石英的损伤特性

利用光学元件激光损伤测试平台,测试了355 nm皮秒激光辐照下熔石英光学元件的初始损伤及损伤增长情况,并通过荧光检测分析了损伤区缺陷。研究结果表明：皮秒激光较高的峰值功率导致熔石英损伤阈值较低,前表面损伤阈值为3.98 J/cm2,后表面损伤阈值为2.91 J/cm2;前后表面损伤形貌存在较大差异,后表面比前表面损伤程度轻且伴随体内丝状损伤;随脉冲数的增加后表面损伤直径增长缓慢,损伤深度呈线性增长;皮秒激光的动态自聚焦和自散焦导致熔石英体内损伤存在细丝和炸裂点重复的现象;与纳秒激光损伤相比,损伤区缺陷发生明显改变。     

355 nm皮秒激光辐照下熔石英的损伤特性

利用光学元件激光损伤测试平台,测试了355 nm皮秒激光辐照下熔石英光学元件的初始损伤及损伤增长情况,并通过荧光检测分析了损伤区缺陷。研究结果表明:皮秒激光较高的峰值功率导致熔石英损伤阈值较低,前表面损伤阈值为3.98 J/cm2,后表面损伤阈值为2.91 J/cm2;前后表面损伤形貌存在较大差异,后表面比前表面损伤程度轻且伴随体内丝状损伤;随脉冲数的增加后表面损伤直径增长缓慢,损伤深度呈线性增长;皮秒激光的动态自聚焦和自散焦导致熔石英体内损伤存在细丝和炸裂点重复的现象;与纳秒激光损伤相比,损伤区缺陷发生明显改变。     

Study of UV laser interaction with gold nanoparticles embedded in silica

In order to resolve problems concerning the understanding and the control of laser-induced damage of silica optical elements, a collaboration between the CEA and different university laboratories has been undertaken. Ultra-pure silica model samples, seeded with gold nanoparticles whose diameter did not exceed 5 nm, were prepared. The aim in using these samples was to observe the mechanism of damage initiation that could be attributed to inclusions of nanometric size. This paper presents the different steps encountered during this study: preparation of the samples, the laser-induced damage tests, the Nomarski and atomic-force microscope observations of this damage and a series of experiments using a time-of-flight mass spectrometer at Argonne National Laboratory. The experimental data are then interpreted, and, in particular, compared to numerical simulations. A very encouraging result is the existence of a pre-damage phase at very low fluences that is not detectable by classical optical devices. The experimental means developed for such model samples should be transposable to the analysis of industrial glasses. Received: 19 July 2002 / Revised version: 23 September 2002 / Published online: 11 December 2002 RID="*" ID="*"Corresponding author. Fax: +33-1/6926-7106, E-mail: florian.bonneau@cea.fr     

Synthesis of nanoclusters by nanosecond laser ablation: Direct simulation Monte Carlo modelling

Collisional processes leading to the formation of nanoparticles in a laser-ablated plume are numerically simulated with the aid of an atomistic-level model based on direct simulation Monte Carlo (DSMC) method. The formation of nanoparticles in nanosecond laser ablation of a mono-atomic target is investigated in the presence of an inert background gas. The DSMC procedure is modified in order to account for numerous plume species and to describe several reactions (i.e., recombination/dissociation, sticking, evaporation) taking place in the plume and affecting the size and spatial distribution of the produced nanoclusters. Calculation results allow us to visualize the nanoparticles and to correlate their space distributions with plume dynamics. In addition, cluster size distributions are investigated at different pressures. The effects of the background gas on cluster formation within the plume are furthermore shown.     

28.4 W 266 nm ultraviolet-beam generation by fourth-harmonic generation of an all-solid-state laser

In this paper, 28.4 W 266 nm ultraviolet-beam generation by fourth-harmonic generation of an all-solid-state laser using a CsLiB₆O₁₀ crystal was reported. A conversion efficiency of 24.7% was obtained.     

Thermal process and surface damage of GaAs induced by 532 nm continuous laser

The thermal damage process of gallium arsenide (GaAs) induced by 532 nm continuous laser is presented in this work. The surface damage in the form of decomposing was detected and determined previous to the melting damage by the real-time observation of surface reflectivity. The evaporation of As induced the decrease of As content in the irradiated surface. The microscopic morphology and composition analysis of the damaged surfaces at different moments during the whole thermal process were performed with an electron probe microscope.     

Plasma plume induced during laser ablation of graphite

The plasma plume induced during ArF laser ablation of a graphite target is studied. Velocities of the plasma expansion front are determined by the optical time of flight method. Mass center velocities of the emitting atoms and ions are constant and amount to 1.7×10⁴ and 3.8×10⁴ m s⁻¹, respectively. Higher velocities of ions result probably from their acceleration in electrostatic field created by electron emission prior to ion emission. The emission spectroscopy of the plasma plume is used to determine the electron densities and temperatures at various distances from the target. The electron density is determined from the Stark broadening of the Ca II and Ca I lines. It reaches a maximum of ∼9.5×10²³ m⁻³ 30 ns from the beginning of the laser pulse at the distance of 1.2 mm from the target and next decreases to ∼1.2×10²² m⁻³ at the distance of 7.6 mm from the target. The electron temperature is determined from the ratio of intensities of ionic and atomic lines. Close to the target the electron temperature of ∼30 kK is found but it decreases quickly to 11.5 kK 4 mm from the target.     

Optical and ultrasonic monitoring of femtosecond laser filamentation in fused silica

Millimeter-long filaments and accompanying luminous plasma and defect channels created in fused silica (FS) by single focused femtosecond laser pulses with supercritical powers were probed in situ using optical imaging and contact ultrasonic techniques. Above the threshold pulse energy E_opt = 5 μJ corresponding to a few megawatt power levels pulses collapse due to self-focusing, producing channels filled by electron-hole plasma and luminescent defects, and exhibits predominantly compressive pressure transients. Analysis of the optical and ultrasonic response versus the laser pulse energy suggests that filamentary pulse propagation in the channels occurs with considerable dissipation of about ∼10 cm⁻¹. The predominant ionization mechanism is most likely associated with avalanche ionization, while the main mechanism of optical absorption is free-carrier absorption via inverse Bremsstrahlung interaction with the polar lattice.     

355 nm纳秒紫外激光辐照下熔石英前后表面损伤的对比研究

为了理解前后表面损伤不对称性的物理内涵, 利用阴影成像技术研究了纳秒紫外激光诱使熔石英光学元件表面损伤的时间分辨动力学过程.研究表明,纳秒紫外激光与熔石英作用过程中前后表面损伤的物理机理是完全不同的.前表面处空气中等离子体和冲击波较强, 等离子体的屏蔽作用抑制了余脉冲能量的沉积, 降低了元件损伤程度.而后表面处等离子体吸收激光能量膨胀, 对后表面冲击作用更为严重, 形成的等离子体电子密度可达到10²³cm^-3以上, 反射部分激光能量与入射的激光余脉冲干涉, 使得 关键词： 熔石英 激光诱使损伤 阴影成像技术 光学元件表面     

355 nm激光作用下熔石英损伤增长

 用355 nm脉冲激光分别辐照位于熔石英前后表面的损伤点,用Mias软件采集了损伤增长的图像并测量了每脉冲辐照后损伤点的面积。实验结果表明：位于熔石英样片后表面的损伤点面积随激光辐照脉冲数呈指数增长关系,而位于前表面的损伤点面积与激光辐照脉冲次数呈线性增长关系。     

Laser impulse coupling at 130 fs

We measured the momentum coupling coefficient C_m and laser-generated ion drift velocity and temperature in the femtosecond (fs) region, over a laser intensity range from ablation threshold to about one hundred times threshold. Targets were several pure metals and three organic compounds. The organic compounds were exothermic polymers specifically developed for the micro-laser plasma thruster, and two of these used “tuned absorbers” rather than carbon particles for laser absorption. The metals ranged from Li to W in atomic weight. We measured time of flight (TOF) profiles for ions. Specific impulse reached record values for this type of measurement and ablation efficiency was near 100%. These measurements extend the laser pulsewidth three orders of magnitude downward in pulsewidth relative to previous reports. Over this range, we found C_m to be essentially constant. Ion velocity ranged from 60 to 180 km/s.     

Two-dimensional ‘hat-scratch’ periodic structures induced by a single femtosecond laser pulse on silica glass

Two-dimensional ‘hat-scratch’ structures are fabricated on silica glass by the interference of three non-coplanar beams originating from a single femtosecond laser pulse. The scanning electron microscope (SEM) characterizations show that the as-formed structures are composed of hat holes and scratch marks. The experimental results indicate that the structures are dependent on the intensity of laser beam. The formation of the two-dimensional ‘hat-scratch’ structures is mainly due to the combined laser ablation effects including ionization, shock wave, plasma expansion, and phase explosion.     

Cooperative Quantum Cutting of Nano-Crystalline BaF2：Tb^3＋, Yb^3＋ in Oxyfluoride Glass Ceramics

We report on cooperative quantum cutting in Tb^3＋- Yb^3＋ codoped glass ceramics. Precipitation of BaF2 nanocrystals is confirmed by XRD and HRTEM analysis. Near-infrared emission due to transition of Yb^3＋ ions under 485 nm excitation indicates cooperative energy transfer from Tb^3＋ to Yb^3＋. The quantum efficiency of this process reaches 145%. The realization of quantum cutting in glass ceramics may have promising applications in solar cells.     

Surface modification of a WTi thin film on Si substrate by nanosecond laser pulses

Interaction of a nanosecond transversely excited atmospheric (TEA) CO₂ laser, operating at 10.6 μm, with tungsten-titanium thin film (190 nm) deposited on silicon of n-type (1 0 0) orientation, was studied. Multi-pulse irradiation was performed in air atmosphere with laser energy densities in the range 24-49 J/cm². The energy absorbed from the laser beam was mainly converted to thermal energy, which generated a series of effects. The following morphological changes were observed: (i) partial ablation/exfoliation of the WTi thin film, (ii) partial modification of the silicon substrate with formation of polygonal grains, (iii) appearance of hydrodynamic features including nano-globules. Torch-like plumes started appearing in front of the target after several laser pulses.     

Absorption and luminescence spectroscopy of fused silica by multiple pulses irradiation at 355 nm

In this work, the effects of laser irradiation on fused silica at 355 nm are investigated by using transient absorption spectroscopy and luminescence spectroscopy. Our result shows that no transient absorption or luminescence in the spectra range from 400 nm to 600 nm is observed when laser energy density is below the damage threshold. When the laser energy density reaches the threshold, an initial damage site will be created. After subsequent laser pulses irradiation, the damage size grows. At the same time, the intensity of the transient absorption and luminescence spectra at the damage site also raises remarkably with the laser pulse number increasing. The absorption band from 420 nm to 520 nm is probably related to the absorption of impurity such as metal ion of iron, cerium and copper. Laser modified fused silica exhibits intense broad luminescence bands due to oxygen-deficiency centers at 444 nm and 580 nm.     

Nanofoaming in the surface of biopolymers by femtosecond pulsed laser irradiation

In this work, the nanostructuring induced in femtosecond (fs) laser irradiation of biopolymers is examined in self-standing films of collagen and gelatine. Irradiation by single 90 fs pulses at 800, 400 and 266 nm is shown to result in the formation of a modified layer with submicrometric size structures. The size and uniformity of the observed features are strongly dependent on irradiation wavelength and on the characteristics of the biopolymer (water content and mechanical strength). Examination of the films by laser induced fluorescence serves to assess the chemical modifications induced by laser irradiation, revealing changes in the emission bands assigned to the aromatic amino acid tyrosine and its degradation products. The results are discussed in the framework of a mechanism involving the generation of large free-electron densities, through multiphoton and avalanche ionization, which determine the temperature and stress distribution in the irradiated volume.