Experimental study on reflection of high-intensity nanosecond Nd:YAG laser pulses in ablation of metals

The total reflectivity of tin and magnesium in ablation by nanosecond Nd:YAG laser pulses in air is studied. It was found that the high initial reflectivity of the studied metals undergoes a significant drop to values of 0.11 for Sn and 0.16 for Mg within a laser fluence range between about 0.8 and 11 J/cm². These reduced reflectivity values remain virtually unchanged with further increasing laser fluence. This study shows that a significant reflectivity decrease of the studied metals is caused by plasma formation in front of the irradiated surface. Below the plasma formation threshold, the reflectivity of the studied metals is observed to be virtually independent of laser fluence, indicating a small role of Drude׳s temperature effect on the reflectivity of the studied samples.     

Femtosecond laser nanostructuring of silver film

In this paper, we report an evolution of surface morphology of silver film irradiated by a 1 kHz femtosecond laser. By SEM observations, it is noted that different nanostructures with respective surface features depend highly on the number of pulses and the laser fluence. Especially when the laser fluence is below the threshold fluence of film breakdown, a textured nanostructure including many nanobumps and nanocavities will appear on the surface of silver film. In order to determine an optimal regime for nanostructuring silver film and to further study the underlying mechanism, we perform a quantitative analysis of laser fluence and pulse number. The results show that this nanostructure formation should be due to a sequential process of laser melting, vapor bubbles bursting, heat stress confinement, and subsequent material redistribution. As a potential application, we find this nanostructured silver film can be used as the active substrate for surface enhanced Raman scattering effect.     

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.     

Direct observation of phase transitions by time-resolved pyro/reflectometry of KrF laser-irradiated metal oxides and metals

New experimental results are obtained by coupling both time-resolved reflectivity and rapid infrared pyrometry under a hemispherical reactor. The heating source KrF laser beam (28 ns, 248 nm) is homogenized and as for probing, a CW He-Ne laser beam (10 mW, 633 nm) is used.Using both methods infrared pyrometry with an IR detector cooled with liquid nitrogen and sensitive in the spectral range 1-12 μm, and time-resolved reflectivity with a rapid photodiode, we were able to study complex thermodynamic transitions with nanosecond time resolution. Three different materials are studied by varying the KrF fluence (energy/surface) from 100 to 2000 mJ/cm²: thin films melting (Au/Ni), the threshold of plasma formation (Ti), and complex liquid phase segregation under semi-conductor state (ZnO). The formation of a liquid Zn film induced by temperature gradient is well evidenced by our signals. Also melting of thin films irradiated by low laser fluences (less than 500 mJ/cm²) translates the typical thermodynamic behavior. Finally, wide fluence dynamic (400-2000 mJ/cm²) is analyzed in the case of Ti surface, and results show two distinguished regimes: first one bellow 1000 mJ/cm² corresponding to the early stage plasma initiation, and second one over 1000 mJ/cm² to the dynamics of plasma expansion.     

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.     

Production of nanostructures on bulk metal samples by laser ablation for fabrication of low-reflective surfaces

Nanostructure formation on bulk noble metals (copper, gold and silver) by a femtosecond laser was studied aiming at the production of low-reflectivity surfaces. The target surface was irradiated with the beam of a 775 nm wavelength and 150 fs pulse duration Ti:sapphire laser. The fluence was in the 16–2000 mJ/cm² range, while the average pulse number was varied between 10 and 1000 depending on the scanning speed of the sample stage. The reflectivity of the treated surfaces was measured with a visible–near-infrared microspectrometer in the 450–800 nm range, while the morphology was studied with a scanning electron microscope. A strong correlation was found between the decreasing reflectivity and the nanostructure formation on the irradiated surface; however, the morphology of silver significantly differed from those of copper and gold. For the two latter metals a dense coral-like structure was found probably as a result of cluster condensation in the ablation plume followed by diffusion-limited aggregation. In the case of silver the surface was covered by nanodroplets, which formation was probably influenced by the ‘spitting’ caused by ambient oxygen absorption in the molten silver followed by its fast release during the resolidification.     

In situ reflectivity investigations of solid/liquid interface during laser backside etching

In situ reflectivity measurements of the solid/liquid interface with a pump-probe setup were performed during laser-induced backside wet etching (LIBWE) of fused silica with KrF excimer laser using toluene as absorbing liquid. The intensity, the temporal shape, and the duration of the reflected light measured in dependence on the laser fluence are discussed referring to the surface modification and the bubble formation.The vaporisation of the superheated liquid at the solid interface causes a considerable increase of the reflectivity and gives information about the bubble lifetime. The alterations of the reflectivity after bubbles collapse can be explained with the changed optical properties due to surface modifications of the solid surface. Comparative studies of the reflectivity at different times and the etch rate behaviour in dependence on the laser fluence show that the in situ measured surface modification begins just at the etch threshold fluence and correlates further with etch rate behaviour and the etched surface appearance. The already observed surface modification at LIBWE due to a carbon deposition and structural changes of the near surface region are approved by the changes of the interface reflectivity and emphasizes the importance of the modified surface region in the laser-induced backside wet etching process.     

Using IR laser radiation for backside etching of fused silica

Laser-induced backside etching of fused silica with gallium as highly absorbing liquid is demonstrated using pulsed infrared laser radiation. The influences of the laser fluence, the pulse number, and the pulse length on the etch rate and the etched surface topography were studied and the results are compared with these of excimer laser etching. The high reflectivity of the fused silica-gallium interface at IR wavelengths results in the measured high threshold fluences for etching of about 3 J/cm² and 7 J/cm² for 18 ns and 73 ns pulses, respectively. For both pulse lengths the etch rate rises almost linearly with laser fluence and reaches a value of 350 and 300 nm/pulse at a laser fluence of about 12 and 28 J/cm², respectively. The etching process is almost free from incubation processes because etching with the first laser pulse and a constant etch rate were observed. The etched surfaces are well-defined with clear edges and a Gaussian-curved, smooth bottom. A roughness of about 1.5 nm rms was measured by AFM at an etch depth of 0.95 μm. The normalization of the etch rates with respect to the reflectivity and the pulse length results in similar etch rates and threshold fluence for the different pulse widths and wavelengths. It is concluded that etching is a thermal process including the laser heating, the materials melting, and the materials etching by mechanical forces. The backside etching of fused silica with IR-Nd:YAG laser can be a promising approach for the industrial usage of the backside etching of a wide range of materials. PACS 81.65.C; 81.05.J; 79.20.D; 61.80.B; 42.55.L     

Radiation effects and pulsed laser deposition of titanium by Nd:Yag laser

A study of Ti laser irradiation and thin film deposition produced by an Nd:Yag pulsed laser is presented. The laser pulse, 9?ns width, has a power density of the order of 10¹⁰?W/cm². The titanium etching rate is of the order of 1?µg/pulse, it increases with the laser fluence and shows a threshold value at about 30?J/cm² laser fluence. The angular distribution of ejected atoms (neutrals and ions) is peaked along the normal of the target surface. At high fluence, the fractional ionization of the plasma produced by the laser is of the order of 10%. Time-of-flight measurements demonstrate that the titanium ions, at high laser fluence, may reach kinetic energies of about 1?keV. Obtained results can be employed to produce energetic titanium ions, to produce coverage of thin films of titanium and to realize high adherent titanium-substrate interfaces. The obtained results can be employed to produce energetic titanium ions, to produce a coverage of thin titanium films on polymers, and to realize highly adherent titanium–substrate interfaces.     

飞秒激光烧蚀硅材料表面形成周期波纹形貌研究

基于Sipe-Drude模型和表面等离子体激元(SPP)的干涉理论分别对单脉冲飞秒激光诱导硅表面形成低频率周期性波纹进行分析研究.探究了波长800 nm、脉宽150 fs的单个飞秒激光烧蚀硅造成不同激发水平下波纹形貌的变化,考虑到材料的光学性质变化(由Drude模型得到的介电常数变化),引入包含双温方程的电子数密度模型.计算结果表明,Sipe-Drude和SPP理论都适用于分析和解释高激发态下周期性波纹,但Sipe-Drude理论更适合分析更为广泛的周期性波纹结构.同时,波纹延伸方向总是垂直于入射激光偏振方向,其空间周期略小于激光波长,并受到入射激光通量的影响.在激光通量为0.38 J/cm~2时,波纹周期达到最小值.另外,还得到了不同入射角度的波纹周期变化情况,并在不同偏振态下随入射角度增大时波纹周期呈现相反的变化趋势.该研究对于理解飞秒激光造成硅表面形成周期结构及其在加工硅材料领域具有重要参考意义.     

Femtosecond laser ablation characteristics of nickel-based superalloy C263

Femtosecond laser (180 fs, 775 nm, 1 kHz) ablation characteristics of the nickel-based superalloy C263 are investigated. The single pulse ablation threshold is measured to be 0.26±0.03 J/cm² and the incubation parameter ξ=0.72±0.03 by also measuring the dependence of ablation threshold on the number of laser pulses. The ablation rate exhibits two logarithmic dependencies on fluence corresponding to ablation determined by the optical penetration depth at fluences below ∼5 J/cm² (for single pulse) and by the electron thermal diffusion length above that fluence. The central surface morphology of ablated craters (dimples) with laser fluence and number of laser pulses shows the development of several kinds of periodic structures (ripples) with different periodicities as well as the formation of resolidified material and holes at the centre of the ablated crater at high fluences. The debris produced during ablation consists of crystalline C263 oxidized nanoparticles with diameters of ∼2–20 nm (for F=9.6 J/cm²). The mechanisms involved in femtosecond laser microprocessing of the superalloy C263 as well as in the synthesis of C263 nanoparticles are elucidated and discussed in terms of the properties of the material.     

基于多形貌银纳米颗粒的多波长相干随机激光研究

采用溶剂热法分别制备了球形银纳米颗粒和多形貌银纳米颗粒,其中球形银纳米颗粒具有400 nm的窄带等离激元共振峰,而多形貌银纳米颗粒的共振区间在400～700 nm之间,将它们分别掺入R6G与PVP的混合溶液中,利用旋涂法在玻璃基板上制备银纳米颗粒嵌入染料掺杂聚合物薄膜随机激光器。采用纳秒脉冲激光进行随机激光泵浦实验,实验结果表明球形银纳米颗粒染料掺杂聚合物薄膜只有自发辐射峰,而多形貌银纳米颗粒染料掺杂聚合物薄膜具有线宽<0.8 nm的相干随机激光发射光谱,其阈值为1.9 mJ·cm-2, 这可能是由于银纳米颗粒的等离激元共振区间与R6G的发射光谱重叠,支持局域等离激元效应的形成,明显的局域场增强有效地改善了与附近分子的相互作用,从而激发了更多的辐射光子,促进了高增益的形成。进一步,利用多形貌银纳米颗粒在银纳米颗粒染料掺杂聚合物薄膜中随机分布的特性,通过改变泵浦位置,实现了20 nm范围内的随机激光输出波长的调控,具体输出范围为590.1～610.4 nm。认为这是由于多形貌银纳米颗粒在不同位置的组成和分布不同,改变了表面等离激元的相互作用和光子的散射能力,从而形成不同的增益效应和不同的封闭光振荡路径。此外,考虑到多形貌银纳米颗粒的共振波长较宽,探究了其用于输出其他颜色光的可能性。以与上述银纳米颗粒R6G染料掺杂聚合物薄膜相似的制备方法,制备了多形貌银纳米颗粒掺杂DCJTB染料聚合物薄膜,并且进行随机激光泵浦实验。结果表明,可以有效的产生波长为675 nm,半高宽<0.8 nm的相干红光随机激光,并且阈值仅为0.98 mJ·cm-2。研究结果在宽带可调谐随机激光器研究以及多色随机激光器研究领域具有重要的参考价值。     

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).     

Reflectivity in femtosecond-laser-induced structural changes of diamond-like carbon film

We report characteristic changes in reflectivity of diamond-like-carbon (DLC) films following irradiation of femtosecond laser pulses at laser fluence around the ablation threshold, where we have observed the formation of periodic nanostructure on the film surface and the modification of bonding structure from DLC to glassy carbon in our recent experiments. The experimental results have shown that the reflectivity change should be a reliable measure to monitor the experimental condition to produce the structural changes, being closely associated with the fundamental physical process to induce these phenomena. PACS 79.20.Ds; 81.40.Tv; 42.62.Cf     

The influence of wavelength in extinction measurements and beam steering in laser-induced incandescence measurements in sooting flames

The accuracy of laser-induced incandescence (LII) measurements is significantly influenced by the calibration process and the laser profile degradation due to beam steering. Additionally, the wavelength used for extinction measurements, needed for LII calibration, is critical and should be kept as high as possible in order to avoid light absorption by molecular species in the flame. The influence of beam steering on the LII measurement was studied in turbulent sooting C₂H₄/air flames at different pressures. While inhomogeneities in the laser profile become smoothed out in time-averaged measurements, especially at higher pressure, the corresponding single-shot beam profiles reveal an increasing effect of beam steering. In the current configuration it was observed that the resulting local laser fluence remains within certain limits (30% to 200%) of the original value. A sufficiently high incident laser fluence can thus prevent the local fluence from dropping below the LII threshold value of approximately 0.3 J/cm² at the cost of increased soot surface vaporization. A spatial resolution in the dimension of the sheet thickness of below 1 mm cannot be guaranteed at increased pressure of 9 bars due to beam steering. A feasibility study in a combustor at technical conditions demonstrates the influence of both effects beam steering and choice of calibration wavelength and led to the conclusion that, however, a shot-to-shot calibration of LII with simultaneously measured extinction can be realized.     

High-fluence he-implantation in Ni trapping,re-emission,and surface modification

Simultaneous measurements have been made of blister formation and gas re-emission during bombardment of Ni with 8–40 keV ³He⁺ at room temperature. It is shown that re-emission and blister formation start at the same critical fluence. An initial peak in the re-emission rate is correlated to a step in the total number of blisters. A more detailed analysis of the experimental data shows that the area contributing to gas re-emission is much larger than the blister area. This suggests the formation of an interconnected layer below the surface in which cracks at blister sites provide gas emission channels to the surface.     

Formation of periodic structures by surface treatments of polyamide fiber: Part I. UV excimer laser irradiation

The processes of UV excimer laser irradiation (both high- and low-fluence) of polyamide fiber were systemically studied, including the surface temperature of the material during the treatment and possible mechanisms for the structure formation. The fluence applied in the high-fluence laser irradiation was above the ablation threshold of the material. The ablation of polymer can be described on the basis of photo-thermal bond breaking within the bulk material. The fluence applied in the low-fluence laser irradiation was far below the ablation threshold of the material. The development of low-fluence laser-induced structures is closely related to the absorption coefficient of the material, the laser fluence used, the polarization of the laser beam, the angle of incidence, and the number of laser pulses applied.     

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     

激光烧蚀Cu靶产生等离子体紫外段发射光谱的研究

利用波长532nm,脉宽15ns的Nd:YAG 激光器作用于Cu靶上,研究了产生等离子体的紫外段（180 nm～300 nm）发射光谱。在局部热力学平衡条件下,采用Boltzmann图表法估算了等离子体的电子温度,得到了电子温度随时间和空间的变化,以及电子温度随激光能量密度的变化。结果显示,随着激光能量的变化,电子温度有一个极大值。随着时间的发展,电子温度先减小,而后增大,接着缓慢减小。随着距靶面距离的增加,电子温度呈下降趋势。     

Interaction of tea CO2 laser light with plasma

High power double discharge type TEA CO₂ laser was used to study laser plasma interaction on carbon target plasma. The maximum output power was 0.3 GW and full width at half maximum intensity was 100 ns. We measured the reflectivity of the laser light at 10.6 μm in wavelength from the carbon plasma. The reflectivity showed a maximum (≈56%) at the laser power intensity of about 1.1 x 10¹⁰ W/cm², and at above this value, the reflectivity decreased. The absorption was introduced effectively above this intensity. The electron density and temperature were also measured.