Dynamics of the ejected material in ultra-short laser ablation of metals

A molecular dynamics model is applied to study the formation and the early stages of ejection of material in ultra-short laser ablation of metals in vacuum. Simulations of the ablation process for iron at a pulse duration of 0.1 ps and at different laser fluences are performed. Different features of the ejection mechanism are observed below, near, and above the ablation threshold. The last is estimated as approximately 0.1 J/cm². The structure of the ablated material is found to depend on the applied laser fluence. The expanded plume consists mainly of large clusters at fluences near to the threshold. With the increase of the laser fluence the presence of the large clusters decreases. Clear spatial segregation of species with different sizes is observed in the direction normal to the surface several tens of picoseconds after the laser pulse onset. The angular distribution of the ejected material is estimated for different regimes of material removal. Above the ablation threshold the distribution is forward peaking. PACS 79.20.Ds; 52.38.Mf; 02.70.Ns; 81.05.Bx     

Identification of non-thermal and thermal processes in femtosecond laser-ablated aluminum

Non-thermal and thermal processes due to femtosecond laser ablation of aluminum (Al) at low, moderate, and high-fluence regimes are identified by Atomic Force Microscope (AFM) surface topography investigations. For this purpose, surface modifications of Al by employing 25 fs Ti: sapphire laser pulses at the central wavelength of 800 nm have been performed to explore different nano- and microscale features such as hillocks, bumps, pores, and craters. The mechanism for the formation of these diverse kinds of structures is discussed in the scenario of three ablation regimes. Ultrafast electronic and non-thermal processes are dominant in the lower fluence regime, whereas slow thermal processes are dominant at the higher fluence regime. Therefore, by starting from the ablation threshold three different fluence regimes have been chosen: a lower fluence regime (0.06–0.5 J cm^?2 single-shot irradiation under ultrahigh vacuum condition and 0.25–2.5 J cm^?2 single-shot irradiation in ambient condition), a moderate-fluence regime (0.25–1.5 J cm^?2 multiple-shot irradiation), and a high-fluence regime 2.5–3.5 J cm^?2 multiple-shot irradiation. For the lower fluence (gentle ablation) regime, around the ablation threshold, the unique appearance of individual, localized Nano hillocks typically a few nanometers in height and less than 100 nm in diameter are identified. These Nano hillock-like features can be regarded as a nonthermal, electronically induced phase transition process due to localized energy deposition as a result of Coulomb explosion or field ion emission by surface optical rectification. At a moderate-fluence regime, slightly higher than ablation threshold multiple-pulse irradiation produces bump-formation and is attributed to ultrafast melting (plasma formation). The high-fluence regime results in greater rates of material removal with highly disturbed and chaotic surface of Al with an appearance of larger protrusions at laser fluence well above the ablation threshold. These nonsymmetrical shapes due to inhomogeneous nucleation, cluster formation, and resolidification of a metallic surface after melting are attributable to slow thermal processes (ps time scale).     

Controlled removal of overpainting and painting layers under the action of UV laser radiation

Laser material removal applied to selective overpaintings and subsequent painting layers detachment was studied in order to select the best cleaning practice of painted artworks. The ablation depth as a function of incident laser fluence/intensity and irradiation pulse number was considered as a reference parameter. We have measured the ablation depth with both a contact microprofilometer and a white light interferometer as a function of laser irradiation parameters. The measurements have evidenced that the ablation depth in our experiments varied between 2 and 100 μm making possible selective removal of painting.     

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.     

Effect of irradiation history on the preparation of laser induced periodic microstructure on polyimide surface

Although UV laser is proved to be an effective tool to prepare microstructure on polymer surface, laser ablation accompanied by the formation of laser induced periodic surface structure (LIPSS) limits its application in many fields. The purpose of this report is to investigate the effect of pre-irradiation in advance, using a low-fluence laser, on the LIPSS formation. The properties of pre-irradiated PI films were characterized by X-ray photoelectron spectroscopy (XPS), surface tension based on the contact angle measurements and UV-vis spectra. It was found that pre-irradiation at low fluence led to the changes in surface property such as chemical components though no LIPSS was formed. As a result, threshold of LIPSS formation on such pre-irradiated PI film decreased and fine LIPSS with deeper amplitude was obtained.     

Femtosecond pulsed laser ablation of 3CSiC thin film on silicon

A femtosecond pulsed Ti:sapphire laser (pulse width=120 fs, wavelength=800 nm, repetition rate=1 kHz) was employed to perform laser ablation of 1-m-thick silicon carbide (3CSiC) films grown on silicon substrates. The threshold fluence and ablation rate, useful for the micromachining of the 3CSiC films, were experimentally determined. The material removal mechanisms vary depending on the applied energy fluence. At high laser fluence, a thermally dominated process such as melting, boiling and vaporizing of single-crystal SiC occurs. At low laser fluence, the ablation is a defect-activation process via incubation, defect accumulation, formation of nanoparticles and final vaporization of boundaries. The defect-activation process reduces the ablation threshold fluence and enhances lateral and vertical precision as compared to the thermally dominated mechanism. Helium, as an assistant gas, plays a major role in improving the processing quality and ablation rate of SiC thin films due to its inertness and high first ionization energy. PACS 79.20.Ds; 42.62.Cf; 42.70.Qs; 61.72; 61.46     

Surface modulation of silicon surface by excimer laser at laser fluence below ablation threshold

Controlled single step fabrication of silicon conical surface modulations on [311] silicon surface is reported utilizing KrF excimer laser [λ=248 nm] at laser fluence below ablation threshold laser fluence. When laser fluence was increased gradually from 0 to 0.2 J/cm² for fixed 200 numbers of shots; first nanopores are observed to form at 0.1 J/cm², then very shallow nanocones evolve as a function of laser fluence. At 0.2 J/cm², nanoparticles are observed to form. Up to 0.15 J/cm² the very shallow nanocone volume is smaller but increases at a fast rate with laser fluence thereafter. It is observed that the net material volume before and after the laser irradiation remains the same, a sign of the melting and resolidification without any ablation.     

飞秒双脉冲激光照射金属薄膜的热行为

通过双温方程对飞秒单脉冲与双脉冲照射金薄膜进行了计算模拟分析,得到了金靶的电子温度和晶格温度随着时间空间的变化。在同样激光能量密度下,单脉冲与双脉冲使得金膜温度的变化表明双脉冲使得更多的激光能量渗透到靶材内部,这些能量可以使得烧蚀深度更深,有利于提高激光烧蚀靶材的效率。计算结果显示随着激光能量密度的增加熔化面深度逐渐增加,单脉冲与双脉冲熔化面深度的变化明显不同。在激光能量密度高于损伤阈值附近,单脉冲的烧蚀深度大于双脉冲的烧蚀深度,随着激光能量密度增加,双脉冲的烧蚀深度将大于单脉冲的烧蚀深度。     

Single-shot ablation threshold of chromium using UV femtosecond laser pulses

Single-shot ablation threshold for thin chromium film was studied using 266 nm, femtosecond laser pulses. Chromium is a useful material in the nanotechnology industry and information on ablation threshold using UV femtosecond pulses would help in precise micromachining of the material. The ablation threshold was determined by measuring the ablation crater diameters as a function of incident laser pulse energy. Absorption of 266 nm light on the chromium film was also measured under our experimental conditions, and the absorbed energy single-shot ablation threshold fluence was \(46 \pm 5\)  mJ/cm². The experimental ablation threshold fluence value was compared to time-dependent heat flow calculations based on the two temperature model for ultrafast laser pulses. The model predicts a value of 31.6 mJ/cm² which is qualitatively consistent with the experimentally obtained value, given the simplicity of the model.     

Aluminum thin film enhanced IR nanosecond laser-induced frontside etching of transparent materials

Laser processing of glass is of significant commercial interest for microfabrication of precision optical engineering devices. In this work, a laser ablation enhancement mechanism for microstructuring of glass materials is presented. The method consists of depositing a thin film of aluminum on the front surface of the glass material to be etched. The laser beam modifies the glass material by being incident on this front-side. The influence of ablation fluence in the nanosecond regime, in combination with the deposition of the aluminum layer of various thicknesses, is investigated by determining the ablation threshold for different glass materials including soda-lime, borosilicate, fused silica and sapphire. Experiments are performed using single laser pulse per shot in an air environment. The best enhancement in terms of threshold fluence reduction is obtained for a 16 nm thick aluminum layer where a reduction of two orders of magnitude in the ablation threshold fluence is observed for all the glass samples investigated in this work.     

Influence of laser fluence and irradiation timing of F2 laser on ablation properties of fused silica in F2-KrF excimer laser multi-wavelength excitation process

A collinear irradiation system of F₂ and KrF excimer lasers for high-quality and high-efficiency ablation of hard materials by the F₂ and KrF excimer lasers’ multi-wavelength excitation process has been developed. This system achieves well-defined micropatterning of fused silica with little thermal influence and little debris deposition. In addition, the dependence of ablation rate on various conditions such as laser fluence, irradiation timing of each laser beam, and pulse number is examined to investigate the role of the F₂ laser in this process. The multi-wavelength excitation effect is strongly affected by the irradiation timing, and an extremely high ablation rate of over 30 nm/pulse is obtained between -10 ns and 10 ns of the delay time of F₂ laser irradiation. The KrF excimer laser ablation threshold decreases and its effective absorption coefficient increases with increasing F₂ laser fluence. Moreover, the ablation rate shows a linear increase with the logarithm of KrF excimer laser fluence when the F₂ laser is simultaneously irradiated, while single KrF excimer laser ablation shows a nonlinear increase. The ablation mechanism is discussed based on these results. Received: 16 July 2001 / Accepted: 27 July 2001 / Published online: 2 October 2001     

Enhancement of the synthesis efficiency of carbon cluster ions by the irradiation of two laser pulses to polymers in vacuum

We investigated the effect of the pre-irradiation of a polymer target in vacuum, using a low-fluence laser pulse, on the synthesis efficiency of carbon cluster ions ejected by laser ablation. A polymer target was irradiated by two laser pulses. The first laser was used for the pre-irradiation, and the second laser was used for ablation. The masses of the ions in the ablation plume were analyzed by time-of-flight mass spectrometry. It was found that the synthesis efficiency of carbon cluster ions was enhanced by the pre-irradiation. The effects of the fluence of the pre-irradiation, the wavelengths of the lasers, and the interval between the oscillations of the two laser pulses on the enhancement of the cluster synthesis are reported. PACS 52.38.Mf; 81.07.-b; 36.40.-c; 61.46.+w     

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.     

Threshold behavior in polyimide photoablation: Single-shot rate measurements and surface-temperature modeling

The ablation rate of Kapton-type polyimide has been measured as a function of incident fluence and excimer laser wavelength using a sensitive quartz-crystal microbalance (QCM). The experiments were performed such that the fluence and the ablated depth were known for each laser pulse, avoiding the need to average rate and fluence data over many pulses. By limiting the investigations to the low-fluence regimes near ablation threshold, high precision and detailed curve shapes were obtained. It was found that the ablation rate increases smoothly and exponentially with increasing fluence for 248, 308, and 351 nm wavelengths. This exponential behavior was modeled using an Arrheniustype thermal rate equation. In contrast, the 193 nm curve is linear in fluence, displays a sharp threshold, and is consistent with a possible photochemical ablation mechanism. Using a sophisticated surface temperature modeling code, the maximum laser induced surface temperature at the fluence at which ablation can first be detected is found to be the same, 850° C, for all four wavelengths. This ablation temperature is significantly higher than the approximately 500° C temperature at which Kapton starts to degrade under isothermal heating conditions.     

Femtosecond uv excimer laser ablation

Experiments on the ablation of polymethylmethacrylate (PMMA) with 300 fs uv excimer laser pulses at 248 nm are reported for the first time. With these ultrashort pulses, ablation can be done at fluences up to five times lower than the threshold fluence for 16 ns ablation of PMMA, and the surface morphology is improved, also for several other materials. A model for ablation is proposed, assuming a non-constant absorption coefficient _eff depending on the degree of incubation of the irradiated material and the intensity of the incoming excimer laser pulse. The agreement between our model and our experimental observations is excellent for 16 ns excimer laser pulses, also predicting perfectly the shape of a pulse transmitted through a thin PMMA sample under high fluence irradiation. Qualitative agreement for 300 fs excimer laser pulses is obtained so far.     

Visualization of nanosecond laser-induced dewetting,ablation and crystallization processes in thin silicon films

In the present work, nanosecond pulsed laser crystallization, dewetting and ablation of thin amorphous silicon films are investigated by time-resolved imaging. Laser pulses of 532 nm wavelength and 7 ns temporal width are irradiated on silicon film. Below the dewetting threshold, crystallization process happens after 400 ns laser irradiation in the spot central region. With the increasing of laser fluence, it is observed that the dewetting process does not conclude until 300 ns after the laser irradiation, forming droplet-like particles in the spot central region. At higher laser intensities, ablative material removal occurs in the spot center. Cylindrical rims are formed in the peripheral dewetting zone due to solidification of transported matter at about 500 ns following the laser pulse exposure.     

Comparison of the transmission behavior of a triazeno-polymer with a theoretical model

The threshold fluence,F _Th, of ablation of a triazeno-polymer was measured in the low fluence range for thin films using conventional UV-spectroscopy. It was found that there is a clearly definedF _Th for 308 nm irradiation between 20 and 25 mJ cm^–2. In the case of 248 nm irradiation, a threshold fluence range between 16 and 32 MJ cm^–2 was found. The ablation rate for both irradiation wavelengths depends on film-thickness. For the XeCl excimer-laser, the point at which the rate becomes independent of thickness was observed to lie at a value which did not correspond to the calculated laser penetration depth, whereas for the KrF laser the independence was not reached within the applied thickness range (up to 0.35 m). Additional transmission measurements have been performed showing that the target transmission at 248 nm increases only slightly, whereas for 308 nm the transmission increases by a factor of approximately 4. This result shows that dynamic target absorption properties are very important for describing the ablation process. The results derived from the transmission studies and etch rates were analyzed theoretically with a two-level model of chromophore absorption. For 248 nm irradiation this model can describe the transmission behavior and the ablation rate. In the case of 308 nm irradiation, it was only possible to match one data set. A good agreement with the experimental transmission ratio does not match the ablation rate and vice versa.     

Ultrashort-pulse laser ablation of indium phosphide in air

Ablation of indium phosphide wafers in air was performed with low repetition rate ultrashort laser pulses (130 fs, 10 Hz) of 800 nm wavelength. The relationships between the dimensions of the craters and the ablation parameters were analyzed. The ablation threshold fluence depends on the number of pulses applied to the same spot. The single-pulse ablation threshold value was estimated to be φ_th(1)=0.16 J/cm². The dependence of the threshold fluence on the number of laser pulses indicates an incubation effect. Morphological and chemical changes of the ablated regions were characterized by means of scanning electron microscopy and Auger electron spectroscopy. Received: 30 May 2000 / Accepted: 31 May 2000 / Published online: 23 August 2000     

Dependence of ablation threshold and LIPSS formation on copper thin films by accumulative UV picosecond laser shots

The ablation threshold and Laser-induced periodic surface structure (LIPSS) formation on copper thin film were investigated using a picosecond laser (Nd:YAG laser: 266 nm, 42 ps, 10 Hz). We show that the ablation threshold varies with respect to the number of laser shots (N) on two different substrates. The single-shot ablation threshold was estimated to be close to 170 ± 20 mJ/cm². The incubation coefficient was estimated to be 0.68 ± 0.03 for copper thin films on silicon and glass substrates. In addition, morphology changes of the ablated regions, in the same spot area, were studied as a function of fluence and number of laser shots. An intermediate structure occurred with a mix of low spatial frequency LIPSS (LSFL), high spatial frequency LIPSS (HSFL) and regular spikes at a fluence F < 250 mJ/cm² and 1,000 < N ≤ 10.000 shots. LSFL was observed with a spatial period close to the irradiation wavelength and an orientation perpendicular to the laser polarization, and HSFL with a spatial period of ～120 nm and a parallel orientation. Lastly, the global relationship between the laser parameters (i.e. fluence and number of shots) and LIPSS formation was established in the form of a 2D map.     

Femtosecond laser micromilling of Si wafers

Femtosecond laser micromilling of silicon is investigated using a regeneratively amplified 775 nm Ti:Sapphire laser with a pulse duration of 150 fs operating at 1 kHz repetition rate. The morphological observation and topological analysis of craters fabricated by single-shot laser irradiation indicated that the material removal is thermal in nature and there are two distinct ablation regimes of low fluence and higher fluence with logarithmical relations between the ablation depth and the laser fluence. Crater patterns were categorized into four characteristic groups and their formation mechanisms were investigated. Femtosecond laser micromilling of pockets in silicon was performed. The effect of process parameters such as pulse energy, translation speed, and the number of passes on the material removal rate and the formation of cone-shaped microstructures were investigated. The results indicate that the microstructuring mechanism has a strong dependence on the polarization, the number of passes and laser fluence. The optimal laser fluence range for Si micromilling was found to be 2-8 J/cm² and the milling efficiency attains its maximum between 10 and 20 J/cm².