Excitation of sodium atoms by 330-nm laser pulses

1/2 ) atoms in a dense sodium vapour irradiated by nanosecond laser pulses tuned near the 3S→4P transition was investigated. It was observed that the population of Na(4P) atoms remained high only within the laser pulse, in spite of the relatively long lifetime of the 4P level (110.ns)The 3P_1/2 level, which is populated as a result of cascade transitions from the higher levels, reached the highest population several nanoseconds after the laser shot. The fast population changes are explained by cascade-stimulated transitions between the excited atomic levels. Received: 16 July 1997/Revised version: 27 October 1997     

脉冲激光辐照氮化硅陶瓷损伤阈值的光谱测量

氮化硅陶瓷具有耐高温、耐腐蚀和耐磨损等优异性能, 可应用于金属材料和高分子材料难以胜任的极端工作环境。但具备这些优良特性的同时也给其加工带来了不便,传统的磨削加工方法效率低,设备损耗严重, 激光辅助加工为其提供了一种新途径。将等离子体光谱法和显微成像法相结合,对脉冲激光辐照氮化硅陶瓷的损伤阈值进行了测量,并分析了损伤机理。实验选用热压烧结氮化硅陶瓷为靶材,参考ISO21254国际损伤阈值测试标准搭建试验系统,采用1-on-1法利用Nd3+∶YAG固体脉冲激光分别在纳秒和微秒脉宽下辐照氮化硅陶瓷,两种脉宽分别选取10个能量密度梯度进行激光辐照,每个能量密度辐照10个点。利用光纤光谱仪采集光谱信息,利用金相显微镜获取显微图像信息,将光谱结果与显微成像结果对比分析, 发现纳秒脉宽下材料一旦损伤光谱上就会出现等离子体峰,通过分析光谱中等离子体峰,元素指认是否含有材料中特征元素即可判断损伤,为了区别空气电离击穿同时测量了空气等离子体光谱对比分析剔除干扰。微秒脉宽下显微图像观察到刚开始损伤时,光谱中只出现较强热辐射谱线并未出现等离子体谱线,进一步增加激光能量密度,光谱中会出现少量等离子体峰,因此不能直接以等离子体峰判断材料损伤阈值。利用金相显微镜观察损伤形貌,纳秒脉宽下在损伤区域内部观察到明显的烧蚀冲击状损伤,光谱呈现出大量等离子体谱线,说明纳秒激光辐照氮化硅损伤机制主要为等离子体冲击波引起的力学损伤效应。微秒脉宽在辐照区域边缘发现热烧蚀痕迹,损伤区内观察到大量熔融物,出现明显热辐射光谱,说明微秒激光辐照氮化硅损伤机制主要是由于长脉宽热积累引起的热损伤效应,随着能量密度增加热辐射谱上叠加有等离子体峰,等离子体峰值强度与损伤程度一致。利用零几率损伤阈值法对两种方法测得结果进行了拟合,分析发现等离子体光谱法更适用于纳秒脉宽下损伤阈值测量,得到结果为0.256 J·cm-2;显微成像法适用于微秒脉宽下损伤阈值测量,得到结果为6.84 J·cm-2。     

Laser-induced damage studies in GaAs

Laser-induced damage studies have been carried out on monocrystal GaAs at 1.06 μm wavelength as a function of pulse repetition rate in the nanosecond regime. The single shot observed laser damage threshold is 0.9 J/cm². It has been found that the damage threshold decreases when the sample is irradiated with large number of pulses. However, the above effect is observed only when the repetition rate is higher than 1 Hz. Various laser damage mechanism theories have been discussed to explain the results.     

Time resolved spectra of optical and electrical transient response induced by nanosecond laser pulses in amorphous AgInSbTe films

The phase transition dynamics of amorphous Ag₈In₁₄Sb₅₅Te₂₃ (AIST) thin films induced by single nanosecond laser pulses were studied by transient optical reflectivity and electrical resistance measurements with nanosecond resolution. Phase transition driven by nanosecond laser pulses can be achieved in a proper fluence range on AIST thin films. The results show that phase transition dynamics driven by nanosecond laser pulses was a multi-stage optical evolution process involving melt, solidification, recalescence, and recrystallion. However, it was found that the real-time responses of optical and electrical signals were quite different under the same irradiated condition. The recalescence process reflected by the second rising of optical reflectivity will not result in obvious changes in electrical resistance. The dependence of saturated time determined by optical and electrical evolution curve on laser pulse fluence was compared and analyzed. A two-dimensional percolation model was employed to explain the difference between electrical and optical transient responses.     

Role of thermal stresses on pulsed laser irradiation of thin films under conditions of microbump formation and nonvaporization forward transfer

This paper presents a theoretical analysis of the processes in thin solid films irradiated by short and ultrashort laser pulses in the regimes of film structuring and laser-induced forward transfer. The regimes are considered at which vaporization of the film materials is insignificant and film dynamics is governed mainly by mechanical processes. Thermoelastoplastic modeling has been performed for a model film in one- and two-dimensional geometries. A method has been proposed to estimate the height of microbumps produced by nanosecond laser irradiation of solid films. Contrary to femtosecond laser pulses, in nanosecond pulse regimes, stress waves across the film are weak and cannot induce film damage. The main role in laser-induced dynamics of irradiated films is played by radial thermal stresses which lead to the formation of a bending wave propagating along the film and drawing the film matter to the center of the irradiation spot. The bending wave dynamics depends on the hardness of the substrate underlying the film. The causes of the receiver substrate damage sometimes observed upon laser-induced forward transfer in the scheme of the direct contact between the film and the receiver are discussed.     

Simulation of pulsed-laser-induced explosive boiling

Bulk evaporation process in absorbing condensed matter irradiated with laser pulses was studied using the one-dimensional thermal model with additional interfaces between different phases. Within this approach, it was shown that the repeated explosive boiling mode can be achieved using nanosecond laser pulses, if the nucleation time is shorter than 0.1 ns. This mode can be observed if the surface pressure is lower than the critical pressure P _c of the liquid-vapor phase transition. The dependences of these processes on the laser pulse intensity and duration, as well as on evaporation kinetics were studied. Explosive boiling and spallation of a transparent liquid film on a pulse-heated absorbing target, as well as the photoacoustic signal in the target before the explosion, were considered.     

Pulsed laser damage of proustite

Pulsed laser damage thresholds have been measured for proustite (Ag₃ As S₃) as the wavelengths 0.694, 1.065, 1.32 and 10.6 μm. The damage thresholds have been found to vary with both the wavelength and duration of the irradiating pulse. At 1.065 μm damage thresholds are 0.38 J/cm² for pulses of duration <50 ns whilst for durations >50 ns a value of 7 MW/cm² is appropriate. The results suggest that damage is initiated by absorbing inclusions approximately 0.6 μm in diameter embedded within the crystals. These inclusions are heated by an incident pulse to cause catastrophic damage of both the surface and interior of an irradiated sample. A model has been developed to enable a study of the thermal behaviour of inclusions irradiated by laser pulses with Gaussian time-dependence to be made.     

Two-photon pumping of random lasers by picosecond and nanosecond lasers

We experimentally demonstrated two-photon pumping of random lasers using picosecond and nanosecond pump lasers. The picosecond laser pumping experiment was performed with 400 ps laser pulses at 770 nm, and the gain media was a Coumarin 480D dye solution doped with TiO₂ nanoparticles. Onset of laser action was observed at a pump laser pulse energy below 500 μJ. The nanosecond laser pumping experiment was performed with 7 ns laser pulses at 1064 nm, and the gain media was a Rhodamine 640 dye solution doped with TiO₂ nanoparticles. Onset of laser action was observed at a pump laser energy ∼18 mJ. Our results suggest that there exists an optimal pulse duration of the pumping laser in two-photon pumped random lasing that leads to minimum photodamage of the gain media and still keeps a high pumping efficiency. PACS 33.50.Dq; 42.55.Mv; 42.55.Zz     

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.     

Nano- and femtosecond UV laser pulses to immobilize biomolecules onto surfaces with preferential orientation

By relying on the photonic immobilization technique of antibodies onto surfaces, we realized portable biosensors for light molecules based on the use of quartz crystal microbalances, given the linear dependence of the method on the laser pulse intensity. Here, we compare the quality of the anchoring method when using nanosecond (260 nm, 25 mJ/pulse, 5 ns, 10 Hz rep. rate) and femtosecond (258 nm, 25 μJ/pulse, 150 fs, 10 kHz rep. rate) laser source, delivering the same energy to the sample with the same average power. As a reference, we also tethered untreated antibodies by means of the passive adsorption. The results are striking: When the antibodies are irradiated with the femtosecond pulses, the deposition on the gold plate is much more ordered than in the other two cases. The effects of UV pulses irradiation onto the antibodies are also analyzed by measuring absorption and fluorescence and suggest the occurrence of remarkable degradation when nanosecond pulses are used likely induced by a larger thermal coupling. In view of the high average power required to activate the antibodies for the achievement of the photonic immobilization technique, we conclude that femtosecond rather than nanosecond laser pulses have to be used.     

Influence of initial micro-porosity of target on material ejection under nanosecond laser pulses

Heating and explosive destruction of the near surface volume of metal with initial micro-porosity under nanosecond laser pulse is simulated. It is shown that presence of initial micro-porosity may influence and modify the ejection mechanisms from melt and from solid phase. Thermal and gas dynamic processes in a gas bubble growing in laser irradiated melt are analysed. Experiments show rather different surface morphology defined by micro-explosions and melt ejection for different metals. Possible explosion of micro-pores and solid particles release under nanosecond laser irradiation is analysed for metals with high melting point. It is shown that the stress attains the values that are close to the damage threshold.     

Self-organization of thin metal films by irradiation with nanosecond laser pulses

Modifications in thin metal films under intensive laser irradiation were studied. Gold, silver, copper, chromium and aluminum films with the thickness of 100 nm were deposited on the glass substrate. Back-side irradiation through the substrate with a burst of nanosecond pulses tightly focused to a line was applied. The film removal threshold with a single pulse F_th was estimated for every material and laser fluence was kept above it in the range of 1.5-3 F_th during experiments. Diverse behavior of the films depending on the metal, the shift between pulses and laser fluence was observed. In chromium, the regular structures were developed in a quite wide range of processing parameters. In gold, three kinds of ripples were observed: transverse (similar to ripples in chromium), longitudinal and a structure of ripples oriented at 60° to each other. The combination of physical properties facilitated the regular assembly of the molten metal in chromium and to some extent in gold.     

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.     

Extracting generalized multiphoton ionization cross-sections from nonperturbative time-dependent calculations: An application in positronium

Ab initio time-dependent (TD) calculations of the behavior of positronium (Ps) under strong subpicosecond laser pulses are presented. The results are compared with results in H through scaling. It is found that a substantial amount of the population can be found in excited states after the pulse. In the perturbative regime, generalized multiphoton ionization cross-sections are extracted from the results of the time-dependent calculations. The generalized cross-sections are used to predict the response of Ps to nanosecond laser pulses at wavelengths of current experimental interest. Beyond the application to Ps, the generality of the method for extracting generalized cross-sections from TD nonperturbative calculations is discussed. Received 8 June 1999     

Theoretical analysis of a Brillouin switch for amplifier decoupling and prepulse suppression in short-pulse high-power laser systems

A switch suited for high-power amplifier chains emitting nanosecond pulses is theoretically investigated. It is based on a two-step Brillouin backscattering process. Gases like N₂ or SF₆ at high pressure are used as the scattering medium. The transmission efficiency is about 50%. The limitation is mainly due to gas breakdown. The capability for amplifier decoupling and prepulse suppression is excellent. Strong pulse steepening favors the generation of ultra-short laser pulses.     

Surface ablation оf aluminum and silicon by ultrashort laser pulses of variable width

Single-shot thresholds of surface ablation of aluminum and silicon via spallative ablation by infrared (IR) and visible ultrashort laser pulses of variable width τ_las (0.2–12 ps) have been measured by optical microscopy. For increasing laser pulse width τ_las < 3 ps, a drastic (threefold) drop of the ablation threshold of aluminum has been observed for visible pulses compared to an almost negligible threshold variation for IR pulses. In contrast, the ablation threshold in silicon increases threefold with increasing τ_las for IR pulses, while the corresponding thresholds for visible pulses remained almost constant. In aluminum, such a width-dependent decrease in ablation thresholds has been related to strongly diminished temperature gradients for pulse widths exceeding the characteristic electron-phonon thermalization time. In silicon, the observed increase in ablation thresholds has been ascribed to two-photon IR excitation, while in the visible range linear absorption of the material results in almost constant thresholds.     

Two-color laser desorption of nanostructured MgO thin films

Neutral magnesium atom emission from nanostructured MgO thin films is induced using two-color nanosecond laser excitation. We find that combined vis/UV excitation, for single-color pulse energies below the desorption threshold, induces neutral Mg-atom emission with hyperthermal kinetic energies in the range of 0.1-0.2 eV. The observed metal atom emission is consistent with a mechanism involving rapid electron transfer to three-coordinated Mg surface sites. The two-color Mg-atom signal is significant only for parallel laser polarizations and temporally overlapped laser pulses indicating that intermediate excited states are short-lived compared to the 5 ns laser pulse duration.     

A time-compensated spectral filter for transform-limited tunable picosecond pulse generation from spectro-temporal-selection dye lasers

Diffraction and transform-limited picosecond tunable pulses are generated from Spectro-temporal-Selection (STS) dye lasers by using a new extra-cavity filter. This filter is based on a grazing-incident grating and arranged in the configuration of a folded dispersive delay line. Thus, it provides both high spectral selectivity and controllable temporal compensation for elimination of pulse broadening. Direct production of diffraction- and transform-limited picosecond dye laser (10 µJ, 50 ps) pulses spectrally adjustable between 398 and 702 nm is demonstrated in a compact device, with 8 ns pump pulses from a nanosecond nitrogen laser.     

Melting and resolidification of gold film irradiated by laser pulses less than 100 fs

The rapid melting and resolidification of gold films irradiated by laser pulses less than 100 fs are investigated using the dual-hyperbolic two-step model. The solid–liquid interfacial velocity in the ultrafast phase change process is obtained by coupling a hyperbolic interfacial energy balance equation and nucleation dynamics. The results are compared with the experimental data for the 28-fs laser. The effects of laser pulse widths and fluences on melting process are investigated. A phase chart of the variations of pulse widths and fluences is established. The relationship between the melting threshold and ablation threshold is also presented.     

Ripple formation in the chromium thin film during laser ablation

The beam of a nanosecond pulse laser tightly focused to a line was applied for the back-side ablation of the chromium thin film on a glass substrate. The stripe ablated with a single laser pulse had sharp edges on both sides and ridges of the melted metal around it. The partially overlapping pulses formed a wide cleaned area with a complicated structure made of the metal remaining from the ridges. Regular structures, ripples, were developed when laser fluence was slightly above the single-pulse removal threshold and the shift between pulses was less than half width of the line ablated with a single laser pulse. The ripples were located periodically (∼4 μm) and were orientated perpendicularly to the long axis of the beam spot. Their orientation did not depend on the laser beam polarization. Different models of the ripple formation in the thin metal film were considered, and instability of the moving vapor-liquid-solid contact line during evaporation of thin liquid films appears to be the most probable process responsible for the observed phenomena. Formation of regular gratings with the unlimited line length was experimentally implemented by using the above-mentioned technique.