SEM and Raman spectroscopy analyses of laser-induced periodic surface structures grown by ethanol-assisted femtosecond laser ablation of chromium

The effect of fluence and pulse duration on the growth of nanostructures on chromium (Cr) surfaces has been investigated upon irradiation of femtosecond (fs) laser pulses in a liquid confined environment of ethanol. In order to explore the effect of fluence, targets were exposed to 1000 pulses at various peak fluences ranging from 4.7 to 11.8?J?cm^–2 for pulse duration of ～25?fs. In order to explore the effect of pulse duration, targets were exposed to fs laser pulses of various pulse durations ranging from 25 to 100?fs, for a constant fluence of 11.8?J?cm^–2. Surface morphology and structural transformations have been analyzed by scanning electron microscopy and Raman spectroscopy, respectively. After laser irradiation, disordered sputtered surface with intense melting and cracking is obtained at the central ablated areas, which are augmented with increasing laser fluence due to enhanced thermal effects. At the peripheral ablated areas, where local fluence is approximately in the range of 1.4–4?mJ?cm^–2, very well-defined laser-induced periodic surface structures (LIPSS) with periodicity ranging from 270 to 370?nm along with dot-like structures are formed. As far as the pulse duration is concerned, a significant effect on the surface modification of Cr has been revealed. In the central ablated areas, for the shortest pulse duration (25?fs), only melting has been observed. However, LIPSS with dot-like structures and droplets have been grown for longer pulse durations. The periodicity of LIPSS increases and density of dot-like structures decreases with increasing pulse duration. The chemical and structural modifications of irradiated Cr have been revealed by Raman spectroscopy. It confirms the formation of new bands of chromium oxides and enol complexes or Cr-carbonyl compounds. The peak intensities of identified bands are dependent upon laser fluence and pulse duration.     

fs Laser surface nano-structuring of high refractory ceramics to enhance solar radiation absorbance

The surface and structural modification of titanium (Ti) has been explored after the interaction of ultrashort laser pulses with the surface target. The targets were exposed by femtosecond Ti: Sapphire laser pulses in liquid (ethanol) and dry (air) environment. In order to explore the effect of pulse energy, the targets were exposed to 1,000 succeeding pulses for various pulse energies ranging from 200 to 500 μJ for pulse duration of 25 fs. SEM analyses were performed for central as well as the peripheral ablated areas of the target. It was found that in the case of ethanol (both for central and peripheral ablated areas) there is a grain growth along with nanoscale pores and dots when the target was irradiated for 200 μJ. For intermediate energies (300–400 μJ), grains of 1–2 μm with distinct boundaries are formed in the central ablated area. Whereas in the peripheral ablated area, laser-induced periodic surface structures (LIPSS) and globules are grown. For the highest pulse energy (500 μJ), distinct grains are observed for both regions. However, in the peripheral area the grains are of bigger size with cracks along the boundaries. In case of ablation in air, in the center of ablated areas, island-like structures with multiple ablative layer or LIPSS and nanoscale spheres are observed both for lower and intermediate pulse energies. For the highest pulse energy only nanoscale LIPSS could be observed. For ablation in air at the peripheral areas, well-defined, laser-induced periodic surface structures are observed for all pulse energies. Raman spectroscopy reveals that the liquid (ethanol) environment forms the carbonyl compounds with the metal and induces C–C stretching vibration, whereas in case of air, hydroxo complexes are formed. It has been found that surface treatment of Ti with ultrashort (25 fs) laser radiation in ethanol environment allows the growth of particular surface structures in the form of grains and simultaneously induces changes in its chemical composition.     

超短脉冲照射下氟化锂的烧蚀机理及其超快动力学研究

研究了超短脉冲激光照射下LiF晶体的破坏机理及其超快动力学过程,利用扫描电镜和原子力显微镜等测试手段,观测了飞秒激光照射下LiF晶体的烧蚀形貌。利用烧蚀面积与激光脉冲能量的对数关系确定了LiF晶体的破坏阈值,并利用非线性玻璃棒展宽脉宽,得到了800nm激光作用下LiF破坏阈值对激光脉宽（50～1000fs）的依赖关系;利用抽运一探针超快探测平台,探测了LiF烧蚀过程中反射率的变化。采用雪崩击穿模型,并根据晶体材料反射率与材料的介电常量的依赖关系,通过数值计算,模拟了材料烧蚀阈值与脉宽的依赖关系及材料激发过程中反射率的变化关系。结果表明,理论结果与实验结果符合较好。讨论了飞秒激光照射下LiF晶体中导带电子数密度的变化规律,并解释了相应的实验结果。     

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.     

Femtosecond laser ablation of polypropylene for breathable film

A polypropylene (PP) film was ablated using a femtosecond laser with a center wavelength of 785 nm, a pulse width of 184 fs and a repetition rate of 1 kHz. Increments of both the pulse energy and the shot number of pulses lead to co-occurrence of photochemical and thermal effect, demonstrated by the spatial expansion of rim on the surface of PP. The shapes of the laser-ablated PP films were imaged by a scanning electron microscope (SEM) and measured by a 3D optical measurement system (NanoFocus). And, the gas and water vapor transmission rate, mechanical properties of PP film micropatterned by fs laser pulses was characterized. Our results demonstrate that a femtosecond pulsed laser is an efficient tool for breathable packaging films in modifying the flow of air and gas, where the micropatterns are specifically tailored in size, location and number of which is easily controlled by laser processing conditions.     

热物性参量对飞秒激光烧蚀金属影响的分子动力学模拟

利用结合双温模型的分子动力学模拟方法,研究了飞秒激光与金属相互作用的烧蚀机制.采用中心波长为800 nm,能量密度从0.043 J·cm~(-2)到0.40 J·cm~(-2)不等,脉宽分别为70 fs和200 fs的激光烧蚀金属镍和铝材料.靶材的温度、原子位型以及内部压力随时间的演化展示了材料热物性参量特性和激光参量对烧蚀结果的影响.结果显示材料电子热传导率对飞秒脉宽激光下的影响仍然较大;对比铝和镍的结果可知,铝的电子晶格耦合系数比镍的小,故电子晶格间的温度梯度持续时间较长;铝的电子热传导系数比镍的大,所以材料上下表面电子温度耦合的时间缩短.铝薄膜表面在能量密度为0.40 J·cm~(-2)激光烧蚀下呈现纳米尺寸的晶体结构.     

Ad-hoc design of temporally shaped fs laser pulses based on plasma dynamics for deep ablation in fused silica

We have analyzed the ablation depth yield of fused silica irradiated with shaped pulse trains with a separation of 500 fs and increasing or decreasing intensity envelopes. This temporal separation value is extracted from previous studies on ablation dynamics upon irradiation with transform-limited 100 fs laser pulses. The use of decreasing intensity pulse trains leads to a strong increase of the induced ablation depth when compared to the behavior, at the same pulse fluence, of intensity increasing pulse trains. In addition, we have studied the material response under stretched (500 fs, FWHM) and transform-limited (100 fs, FWHM) pulses, for which avalanche or multiphoton ionization respectively dominates the carrier generation process. The comparison of the corresponding evolution of the ablated depth vs. fluence suggests that the use of pulse trains with decreasing intensity at high fluences should lead to enhanced single exposure ablation depths, beyond the limits corresponding to MPI- or AI-alone dominated processes.     

飞秒激光烧蚀镍钛形状记忆合金的蚀除机理

结合双温模型的分子动力学模拟方法,研究了飞秒激光脉冲辐照B2结构镍钛合金时烧蚀阈值附近的靶材蚀除机制,数值模拟了中心波长为800nm,脉宽为100fs,能量密度为25~50mJ/cm2的激光与90nm厚B2结构镍钛合金薄膜相互作用过程。确定了脉宽为100fs的脉冲激光与镍钛形状记忆合金相互作用的烧蚀阈值,发现烧蚀阈值条件下,靶材的蚀除机制是单纯基于应力作用的机械破碎;烧蚀阈值附近,未蚀除靶材受热影响发生无序化相变的区域较小,且随激光能量密度的降低而减小。提高激光功率密度,烧蚀同时呈现热机械蚀除和机械破碎机制。     

The growth of nanoscale periodic and dot-like structures on the surface of stainless steel with femtosecond laser pulses in the dry and wet ambient environment

The present work deals with growth of nanoscale periodic and dot-like structures on the surface of stainless steel (SS) by the irradiation of femtosecond laser pulses. For this purpose Ti: Sapphire femtosecond laser pulses (wavelength of 800 nm, pulse length of 25 fs and pulse repetition rate of 1 kHz) were employed in a dry (air) and liquid confined (deionized water and ethanol) environments. The targets were exposed to 1000 succeeding pulses for various fluences ranging from 50 to 150 mJ?cm^?2. Nanoscale structures including ripples, and dots were observed by SEM analysis. The growth and dependence of structure-formation on the ambient environment and laser fluence in both central as well as peripheral ablated areas is systematically investigated. The development of nanostructures and nanoripples is correlated with structural analysis carried out by micro Raman spectroscopy.     

Ultrafast two-color ablation of fused silica

Two ultrafast laser pulses at the fundamental Ti:sapphire laser wavelength of 800 nm and the second harmonic at 400 nm were used to study the temporal evolution of the transmissivity in fused silica and resulting material ablation. It was observed that there was a sharp drop in the transmissivity of the probe pulse at zero delay between the two pulses, indicating that there was enhanced absorption/reflection due to the creation of defect states or free electron plasma by the pump pulse. Subsequent atomic force microscopy measurements of the ablated holes revealed that the ablated volume increased by about 50% when the separations of the two pulses are within 300 fs. Two-color machining of channels at the surface also showed a similar increase in the machined depth and width when the pulses are overlapped in time. PACS 52.38.Mf; 78.47.+p; 79.20.Ds     

超短激光脉冲对宽带光学物质的微加工

通过讨论超快飞秒激光脉冲和长脉冲宽度的激光脉冲紧导致宽能隙透明电介质的损伤机理和比较超短激光脉冲与长激光脉冲对宽能隙透明电介质的损伤程度，得出超短激光脉冲是一种可对透明宽带电介质进行加工的有效工具的结论。当波长为800nm，脉冲宽度为150fs的激光脉冲紧聚焦到不同的宽能隙透明电介质（K9玻璃和ZK6玻璃）体内时，可制作不同光栅常数的光栅，并在波长为635nm的He-Ne连续激光的垂直照射下，对光栅的远场相对衍射效率和光栅的衍射效率进行了测量。     

富勒烯有机-无机杂化材料的非共珍三阶非线性光学特性

采用中心波长800 nm、脉宽30 fs的超短激光脉冲,通过飞秒光开关技术(Optical Kerr Shutter,OKS)对富勒烯有机-无机杂化材料的飞秒超快非线性特性进行了实验研究.获得270 fs的开关时间,所得的富勒烯有机-无机杂化材料的三阶非线性系数X~(3)约为4.5×10~(-4) esu,比C_(60)分子的三阶非线性系数X~(3)高一个数量级.通过实验测定的光克尔信号强度与激发光和探测光偏振方向夹角的依赖关系表明:30 fs的超短激光脉冲激发富勒烯有机-无机杂化材料的克尔信号主要是源于光诱导双折射效应,而非用200 fs的超短激光脉冲时来自瞬态栅的自衍射效应.     

Laser ablation of polymers using 395 nm and 790 nm femtosecond lasers

We compared a Ti:sapphire fs laser (790 nm) with a second harmonics (395 nm) fs laser, and then mixed them for ablating polyethylene (PE). Compared to the 790 nm fs laser, the 395 nm fs laser harmonics could etch PE faster. However, isolated carbon was formed on the ablated surface, in addition to C=O and C=C-H bonds. When we mixed a faint beam of the 395 nm fs laser harmonics with the 790 nm fs laser, the etching depth became even deeper. Moreover, the chemical composition of the ablated surface remained unchanged. At a total laser fluence of 80 mJ/cm², the most suitable laser fluences for the 395 nm fs laser harmonics and the 790 nm fs laser were found to be approximately 2 and 78 mJ/cm² respectively. PACS 81.65.Cf     

富勒烯有机-无机杂化材料的非共珍三阶非线性光学特性

采用中心波长800 nm、脉宽30 fs的超短激光脉冲,通过飞秒光开关技术（Optical Kerr Shutter,OKS）对富勒烯有机-无机杂化材料的飞秒超快非线性特性进行了实验研究.获得270 fs的开关时间,所得的富勒烯有机-无机杂化材料的三阶非线性系数χ(3)约为4.5×10－14 esu,比C60分子的三阶非线性系数χ(3)高一个数量级.通过实验测定的光克尔信号强度与激发光和探测光偏振方向夹角的依赖关系表明：30 fs的超短激光脉冲激发富勒烯有机-无机杂化材料的克尔信号主要是源于光诱导双折射效应,而非用200 fs的超短激光脉冲时来自瞬态栅的自衍射效应.     

PMP泡沫的飞秒激光烧蚀及切割方法

对密度为90 mg/cm3的PMP泡沫材料的飞秒激光烧蚀结果进行了分析,推导出该材料在脉宽50 fs、波长800 nm、重复频率为1000 Hz的飞秒激光作用下的蚀除阈值为0.91 J/cm2（100个激光脉冲）,获得了烧蚀直径分别随激光功率、脉冲数及聚焦物镜数值孔径的变化规律。相同飞秒激光加工系统下,对比了铜箔上获得的烧蚀形状,确定了PMP泡沫材料本身的多孔洞及其分布不均匀是造成烧蚀区域的形状不规则的重要因素。PMP泡沫在较高能量或是较长时间的飞秒激光作用下,烧蚀区域发生碳化的原因是由热作用引发的。提出了一种基于激光束耦合的飞秒激光切割厚度大于1 mm的薄膜-泡沫材料的方法,并获得了切割厚度大于1.5 mm、切割侧壁与光束光轴夹角小于5、切割面整洁的薄片。     

Influence of the laser-spot diameter on photo-ablation rates

The dependence of the ablation rate of various materials on the laser spot diameter on the sample surface has been investigated. The experiments have been performed with excimer lasers at the wavelengths 193, 248 and 308 nm. Polymers, aluminum oxide ceramics, and glasses have been ablated under vacuum and ambient atmosphere conditions. In general, all materials show a more or less pronounced increase of the ablation rate with decreasing spot diameter in the range of 10–200 μm if pulses with nanosecond pulse durations are applied. For ultrashort pulses (500 fs) at 248 nm this diameter dependence is not observed. The expansion of the ablation plume over areas of different size seems to be the main reason for this effect.     

Time-resolved investigations of plasma and melt ejections in?metals by pump-probe shadowgrpahy

Ablation of bulk metals (Al, Cu) has been investigated in situ by means of high-resolution pump-probe photography using pump laser radiation of pulse duration t _p=80 fs, at wavelength of 820 nm. Depending on material-specific parameters, qualitatively different ablation phenomena have been observed. Structural analysis by electron and optical microscopies reveals rosette-like surface structures showing the morphology of the ablated regions. The temporal development of the ablation dynamics can be conditionally categorized into different characteristic time regions. Particularly, laser induced melt injection has been observed in the time range of 700 ns to 1.1 μs after the initial laser-metal interaction.     

Microablation with ultrashort laser pulses

This paper reports the micromachining results of different materials (Al, Si, InP and fused silica) using a Ti : sapphire laser at the wavelength of 800 and 267 nm with variable pulse lengths in the range from 100 fs to 10 ps. The hole arrays with a diameter up to a few μm through microdrilling are presented. We discussed how an effective suppression of the thermal diffusion inside the ablated materials and an effective microablation could be realized. If the laser fluence is taken only slightly above the threshold, a hole array can be drilled with diameters even smaller than the wavelength of the laser. Some examples are presented in the paper.     

Generation of higher-order harmonics of chirped radiation from a titanium-sapphire laser in plasma generated by pulses of different durations

The frequency conversion of laser radiation in plasma created by pulses of different durations under conditions of the chirp variation of the radiation to be converted is investigated. It is shown that the chirp variation of the laser pulse during the generation of higher-order radiation harmonics of the femtosecond laser leads to a considerable change in the brightness, wavelength shift, and maximal order of generated harmonics. The long-and short-wavelength shifts of harmonics observed in these studies are attributed to the manifestation of a considerable concentration of free charge carriers in the plasma, as well as the self-modulation of the laser pulse. The generation of plasma by pulses whose durations vary from 160 fs to 20 ns is considered and it is shown that the generation efficiency of harmonics depends to a greater extent on the energy of the heating prepulse than on its intensity on the surface of a target to be ablated. The effect that the atomic number of the target has on the formation of optimal plasma at different delays between the heating prepulse and the femtosecond pulse to be converted is discussed.     

Study of x-ray emission enhancement via a high-contrast femtosecond laser interacting with a solid foil

We observed the increase of the conversion efficiency from laser energy to Kalpha x-ray energy (eta(K)) produced by a 60 fs frequency doubled high-contrast laser pulse focused on a Cu foil, compared to the case of the fundamental laser pulse. eta(K) shows a strong dependence on the nonlinearly modified rising edge of the laser pulse. It reaches a maximum for a 100 fs negatively modified pulse. The hot electron efficient heating leads to the enhancement of eta(K). This demonstrates that high-contrast lasers are an effective tool for optimizing eta(K), via increasing the hot electrons by vacuum heating.