Enhancement of resolution and quality of nano-hole structure on GaN substrates using the second-harmonic beam of near-infrared femtosecond laser

By using a second harmonic of near infrared femtosecond (fs) laser (λ=387 nm, 150 fs) with high NA objective lens, fabrication resolution has been greatly improved in nano-fabrication of wide band-gap semiconductor gallium nitride (GaN). We have carried out a wet-chemical-assisted fs laser ablation method, in which the laser beam is focused onto a single-crystal GaN substrate immersed in a concentrated hydrochloric (HCl) acid solution. A two-step processing involving irradiation with a fs laser beam in air followed by wet chemical treatment is also performed for comparison. In the wet-chemical-assisted ablation, theoretical diameters of ablation craters are calculated as a function of pulse energy by assuming that the reaction is based on two-photon absorption. In lower energy, the calculated curve is close to the experimental value, while the actual measured diameters in the region of higher energy are larger than calculated values. In the condition of the highest fabrication resolution, we obtained ablation craters smaller than 200 nm at full width at half maximum. We have also demonstrated the fabrication of two-dimensional (2D) periodic nanostructures on surface of a GaN substrate using the second harmonic single fs-laser pulse. Uniform ablation craters with the size as small as 410 nm in diameter are arranged with a periodicity of 1 μm. Such structures are applicable to 2D photonic crystals which improve the light extraction efficiency for blue LEDs in the near future.     

Thermal characteristics of double-layer thin film target ablated by femtosecond laser pulses

Thermal characteristics of tightly-contacted copper--gold double-layer thin film target under ablation of femtosecond laser pulses are investigated by using a two-temperature theoretical model. Numerical simulation shows that electron heat flux varies significantly on the boundary of copper--gold film with different maximal electron temperature of 1.15×10³ K at 5 ps after ablating laser pulse in gold and copper films, which can reach a balance around 12.6 ps and 8.2 ps for a single and double pulse ablation, respectively, and in the meantime, the lattice temperature difference crossing the gold--copper interface is only about 0.04×10³ K at the same time scale. It is also found that electron--lattice heat relaxation time increases linearly with laser fluence in both single and double pulse ablation, and a sudden change of the relaxation time appears after the laser energy density exceeds the ablation threshold.     

飞秒激光在空气和水中对硅片烧蚀加工的实验研究

采用1 kHz,800 nm,50 fs—24 ps的钛宝石激光脉冲对单晶硅样品在空气和水溶液环境中的烧蚀加工特性进行了研究.实验观察到了超短脉冲激光在空气氛围中烧蚀形成的双层环状结构,分析揭示了加工区域中心和边缘的烧蚀物理机制分别为热熔化和库仑爆炸,并测量了双层环状结构半径随入射激光能量、脉冲数及持续时间等的变化关系,结果表明获取较大深-宽比的加工效果需选择小能量脉冲激光的多次作用.在水溶液环境中,实验发现飞秒激光在样品表面诱导产生了亚微米量级的多孔状结构,而皮秒激光则更容易实现对硅表面的非热性去除.这是由于激光诱导的光机械应力和空泡效应随脉冲宽度变大而增强所致,在实验上确立了区分这两种不同加工状态的临界脉冲宽度. 关键词： 飞秒激光 硅片 激光加工     

Talbot effect under illumination of double femtosecond laser pulses

The Talbot effect under illumination of double femtosecond laser pulses has been reported. Spectrums of double femtosecond laser pulses with phase differences are quite different from that of one single femtosecond laser pulse. Therefore, the Talbot images of the double femtosecond laser pulses with phase differences are different from that of one single femtosecond laser pulse. Specifically, for the phase difference corresponding to π, the Talbot image shows the largest difference from that of one single pulse. Experimental results are in good agreement with the theoretical analysis. The behaviors of Talbot images under double femtosecond laser pulses illumination cannot be obtained under one femtosecond laser pulse, monochromatic or polychromatic light illumination. Therefore, it is a new interesting optical phenomenon for the Talbot effect which should have potential applications.     

A detailed study through the focal region of near-threshold single-shot femtosecond laser ablation nano-holes in borosilicate glass

A detailed study of the morphology of nano-craters drilled in borosilicate glass by single shot femtosecond laser ablation near the ablation threshold has been performed by scanning electron microscopy, atomic force microscopy and scanning electron microscopy imaging after focused ion beam sectioning. The influence of the numerical aperture (NA = 0.4 and 0.8), the pulse energy (16 nJ < E_p < 600 nJ) and the position of the specimen surface into the focal region were systematically investigated, leading to nanometric or micrometric scales in every spatial dimension. The nanocrater’s size is not restricted by the diffraction limit but determined by the laser pulse stability and the material properties. If the beam is focused inside the glass, two craters are drilled, shaping very distinct morphologies. Their dimensions have been studied in details and different relationships have been proposed for the evolutions of the depths and of the various diameters of these craters as functions of the pulse energy, the numerical aperture and the position of specimen surface in the beam-material interaction region. It is suggested that the long, thin conical profile with very high aspect ratio of the secondary craters is due to a spontaneous reshaping of the beam which transforms the incoming Gaussian pulse into a Gaussian-Bessel pulse. As proposed in the developed model the geometry of the second craters seems to be connected with the one of the main craters.     

飞秒激光烧蚀LiNbO3晶体的形貌特征与机理研究

采用了不同能量的单脉冲和多脉冲飞秒激光对LiNbO₃晶体进行烧蚀，并刻蚀了表面衍射型光栅.通过扫描电镜和原子力显微镜观察了烧蚀点的形貌特征，首次发现利用单束飞秒激光脉冲对LiNbO₃晶体烧蚀，可以得到超衍射极限的烧蚀点，当聚焦光斑直径约为2μm、能量为170nJ的单脉冲飞秒激光作用时，烧蚀点的直径约为400nm，100nJ，17个脉冲作用时烧蚀点的直径约为800nm.同时可以观察到在能量较低的多脉冲飞秒激光作用下， LiNbO₃晶体呈现出大约200nm周期性分布的波纹状结构.实验结果表明，选择合适参数的飞秒激光脉冲可以对LiNbO₃晶体进行超衍射极限加工，这对于利用飞秒激光制作LiNbO₃基质的微纳光电子器件有十分重要的意义.     

Time-resolved shadowgraphs and morphology analyses of aluminum ablation with multiple femtosecond laser pulses

Aluminum ablation by multiple femtosecond laser pulses is investigated via time-resolved shadowgraphs and scanning electron microscope(SEM) images of the ablation spot. The spatial distribution of the ejected material and the radius of the shock wave generated during the ablation are found to vary with the increase in the number of pulses. In the initial two pulses, nearly concentric and semicircular stripes within the shock wave front are observed, unlike in subsequent pulses. Ablation by multiple femtosecond pulses exhibits different characteristics compared with the case induced by single femtosecond pulse because of the changes to the aluminum target surface induced by the preceding pulses.     

Femtosecond pulsed laser ablation with spatial filtering

With the rise in demand for miniaturized features with better acute edge acuity and negligible thermal damage zone, one of the key vital areas lies in the refinement of the quality of the laser beam itself. Spatial filter is routinely used in optical micromachining systems to smoothen the Gaussian profile of the machining spot in order to obtain a feature of the desired quality. However, its profile smoothening effect has never been investigated for femtosecond pulsed laser micromachining process since the extremely high peak power of femtosecond pulses will cause damage on the filtering aperture of spatial filter. During the development of an acousto-optical micromachining system using femtosecond pulses, we found that if the damage of the filtering aperture can be circumvented, spatial filter can improve the machining quality of femtosecond pulse ablation, especially when ablation is conducted at low-fluency range (just above the ablation threshold fluency). In this paper, we investigate and demonstrate both the improvement and potential that beam refinement can bring about. In our experiment, a series of test patterns were ablated with a 400 nm second-harmonic Ti:Sapphire femtosecond laser of 150 fs duration at varying pulse energy ranging from 31 to 39 nJ. The specimen used in the experiment is a platinum- (Pt) sputtered coating of 100 nm thickness on a quartz substrate. The results show a significant improvement in the constancy of the shape as well as the size of ablated feature, revealing an improved beam profile and beam energy distribution due to spatial filtering.     

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.     

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.     

Experimental investigation of ablation efficiency and plasma expansion during femtosecond and nanosecond laser ablation of silicon

Femtosecond laser (Ti:sapphire, 100 fs pulse duration) ablation of silicon in air was compared with nanosecond laser (Nd:YAG, 3 ns pulse duration) ablation at ultraviolet wavelength (266 nm). Laser ablation efficiency was studied by measuring crater depth as a function of pulse number. For the same number of laser pulses, the fs-ablated crater was about two times deeper than the ns-crater. The temperature and electron number density of the laser-induced plasma were determined from spectroscopic measurements. The electron number density and temperature of fs-induced plasmas decreased faster than ns-induced plasmas due to different energy deposition mechanisms. Images of the laser-induced plasma were obtained with femtosecond time-resolved laser shadowgraph imaging. Plasma expansion in both the perpendicular and the lateral directions were compared. PACS 52.38.Mf; 52.30.-q     

双飞秒激光脉冲诱导击穿光谱增强特性研究

在大气环境中,以钴为样品,通过单脉冲飞秒激光诱导击穿光谱及共轴双飞秒脉冲激光诱导击穿光谱的对比实验,研究了双脉冲激光诱导击穿光谱的谱线增强机制,测量了双脉冲激光诱导击穿光谱随脉冲时间间隔的变化趋势。结果表明,在最优化的脉冲时间间隔条件下,双脉冲激光诱导等离子体光谱获得明显增强。进一步,通过线性Boltzmann法得出了电子温度随脉冲时间间隔的演化,发现了谱线增强因子和电子温度随脉冲时间间隔呈现出相同的演化趋势,并经历两个明显的变化过程,得出了谱线信号强度的增强依赖于电子温度升高的结论。     

Threshold effect in femtosecond laser induced nanograting formation in glass: influence of the pulse duration

Recently, femtosecond laser direct writing in porous glass is emerging as a powerful technique for building arbitrary 3D hollow micro/nanostructures in bulk glass materials. In this study, we investigate the pulse duration dependence of laser intensity window for inducing a single nanocrack inside porous glass by femtosecond laser direct writing. We find that the window for a single nanocrack increases with the pulse duration, while the roughness of side walls in the nanocracks becomes higher for pulses longer than ~300 fs. When the femtosecond laser pulses of an optimized duration of ~200 fs are chosen, a sufficiently broad range of laser intensity (~44 % of the structuring threshold) for creating a single nanocrack can be obtained, while smooth sidewalls required by nanofluidic applications can still be maintained. The reported results will be beneficial not only for the development of the 3D femtosecond laser micro/nanostructuring techniques, but also for gaining a deeper understanding of the physical mechanism behind the nanograting formation induced by femtosecond laser irradiation in glass and other transparent materials.     

Morphology studies of the metal surfaces with enhanced absorption fabricated using interferometric femtosecond ablation

Recently, the enhancing of bulk metals optical absorption with focused femtosecond pulses was demonstrated. This absorption enhancement is caused by different nano- and micro-structures which are formed during laser ablation with ultrashort pulses. In this paper we study the evolution of the surface structures using interferometric ablation and compare it to normal fs-ablation. Previously we have shown that interferometric femtosecond ablation is an efficient method to fabricate absorbing metal surfaces. In this study we ablated large areas of hole-array structures with different pulse numbers in polished stainless steel and copper samples. The evolution of surface morphology and the depth of the holes for these structured surfaces are presented. In addition, the reflectance of laser generated surface structures are measured at the wavelength range of 200–2300 nm using a standard spectrophotometer.     

Nanosecond and femtosecond ablation of La0.6Ca0.4CoO3: a comparison between plume dynamics and composition of the films

Thin films of La_0.6Ca_0.4CoO₃ were grown by pulsed laser ablation with nanosecond and femtosecond pulses. The films deposited with femtosecond pulses (248 nm, 500 fs pulse duration) exhibit a higher surface roughness and deficiency in the cobalt content compared to the films deposited with nanosecond pulses (248 nm, 20 ns pulse duration). The origin of these pronounced differences between the films grown by ns and fs ablation has been studied in detail by time-resolved optical emission spectroscopy and imaging. The plumes generated by nanosecond and femtosecond ablation were analyzed in vacuum and in a background pressure of 60 Pa of oxygen. The ns-induced plume in vacuum exhibits a spherical shape, while for femtosecond ablation the plume is more elongated along the expansion direction, but with similar velocities for ns and fs laser ablation. In the case of ablation in the background gas similar velocities of the plume species are observed for fs and ns laser ablation. The different film compositions are therefore not related to different kinetic energies and different distributions of various species in the plasma plume which has been identified as the origin of the deficiency of species for other materials.     

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。     

Guidelines for efficient direct ablation of dielectrics with single femtosecond pulses

We provide guidelines to femtosecond laser users to select ad hoc laser parameters, namely the fluence and pulse duration, in the context of the development of ablation processes at the surface of dielectrics using single femtosecond pulses. Our results and discussion are based on a comprehensive experimental and theoretical analysis of the energy deposition process at the surface of fused silica samples and of their postmortem ablation characteristics, in the range of intensities from 10¹³ to 10¹⁵ W/cm². We show experimentally and numerically that self-induced plasma transient properties at the pulse timescale dramatically determine the efficiency of energy deposition and affect the resulting ablation morphology. In practice, we determine that the precise measurement of two characteristic fluence values, namely the laser-induced ablation threshold F _th,LIAT and the fluence F _opt for maximum ablation efficiency, are only required to qualify the outcomes of laser ablation at the surface of a dielectric in an extended range of applied fluence.     

Deep drilling on a silicon plate with a femtosecond laser: experiment and model analysis

The ablation rate when drilling fine holes having large aspect ratios in silicon substrates with femtosecond laser pulses was estimated from mechanically ground cross sections of the ablated holes. The ablation rate shows a dramatic change at the depth at which the laser pulse reaches a certain fluence, which is nearly constant when the initial laser fluence was varied from 14.5 to 59.4 J/cm². The ablation rate, threshold fluence, in three fluence domains, and the transition fluences at which the ablation rate shows a dramatic change, were derived. However, when a pulse energy of 200 μJ was used a much greater ablation rate was obtained, suggesting that another fluence domain for larger ablation rates exists. The experimentally obtained hole depths as a function of shot numbers were reproduced by a theoretical model, which incorporates laser pulse attenuation in the holes that is the same as that in waveguides for some attenuation coefficient and ablation rates for three fluence domains. PACS 42.62.-b; 42.65.Re; 78.40.Fy; 78.47.+p; 81.20.Wk     

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.     

Thermal behavior of thin metal films irradiated by shaped femtosecond pulse sequences laser

A numerical solution of the two-temperature model has been performed up to the shaped femtosecond pulse sequences heated metal target. The two-temperature model is used to analyze the shaped femtosecond pulse sequences with the following major conclusions. We confirm the distinctly different results on the different shaped femtosecond pulse sequences. As the number of shaped femtosecond pulses increases, the nonequilibrium state between electrons and phonons gradually disappears, the highest transient electron temperature is lowered and the thermolization time is prolonged, the electron heat conductivity remains higher because of the effect of incubation on the electron temperature, which preserves the advantages of ultrashort lasers. The shaped femtosecond pulse sequences can increase the efficiency in ablation and micromachining.