Nanospallation induced by an ultrashort laser pulse

A femtosecond laser pulse with power density of 10¹³ to 10¹⁴ W/cm² incident on a metal target causes ablation and ejection of the surface layer. The ejected laser plume has a complicated structure. At the leading front of the plume, there is a spall layer where the material is in a molten state. The spall layer is a remarkable part of the plume in that the liquid-phase density does not decrease with time elapsed. This paper reports theoretical and experimental studies of the formation, structure, and ejection of the laser plume. The results of molecular dynamics simulations and a theoretical survey of plume structure based on these results are presented. It is shown that the plume has no spall layer when the pulse fluence exceeds an evaporation threshold F _ev. As the fluence increases from the ablation threshold F _a to F _ev, the spall-layer thickness for gold decreases from 100 nm to a few lattice constants. Experimental results support theoretical calculations. Microinterferometry combined with a pump-probe technique is used to obtain new quantitative data on spallation dynamics for gold. The ablation threshold is evaluated, the characteristic crater shape and depth are determined, and the evaporation threshold is estimated.     

Analysis of plume deflection in the silicon laser ablation process

Changes in target surface morphology and ablation plume direction have been experimentally observed during the initial stages of the silicon laser ablation process. A relationship between both phenomena can be observed upon analysing the temperature field induced by the laser beam in a rough surface material. Theoretical studies on the deflection of the ablation plume are presented. These analyses are based on the hypothesis that particles that reach evaporation temperature will exit normally to the target surface with a velocity that is proportional to the surface temperature and the amount of the ablated material. Numerical solutions and experimental results of laser ablation process of silicon targets are found to agree with theoretical studies. PACS 42.25.Lc; 79.20.Dc; 02.70.Dc     

切向气流作用下玻璃纤维复合材料的激光辐照效应

实验研究了样品表面有切向空气气流、切向氮气气流和无气流时,976 nm连续激光对玻璃纤维增强E-51环氧树脂复合材料的辐照效应。结果表明:无气流时,喷出的热分解产物会对入射激光产生屏蔽作用;有气流时,激光对玻璃纤维的破坏方式是其升温熔化后再被切向气流带走;当激光功率密度较低时,切向空气气流以加强样品表面的对流冷却作用为主,不利于激光对玻璃纤维复合材料的破坏;当激光功率密度较高时,切向空气气流以降低屏蔽作用和提供氧气助燃为主,有利于激光对玻璃纤维复合材料的破坏。三种气流状态下,质量损失随功率密度呈现单调增加趋势,当入射激光功率密度在100~600 W/cm2范围内,随着功率密度的增大,激光能量的利用效率逐渐增大并趋于稳定。     

A multi-step reaction model for ignition of fully-dense Al-CuO nanocomposite powders

A multi-step reaction model is developed to describe heterogeneous processes occurring upon heating of an Al-CuO nanocomposite material prepared by arrested reactive milling. The reaction model couples a previously derived Cabrera-Mott oxidation mechanism describing initial, low temperature processes and an aluminium oxidation model including formation of different alumina polymorphs at increased film thicknesses and higher temperatures. The reaction model is tuned using traces measured by differential scanning calorimetry. Ignition is studied for thin powder layers and individual particles using respectively the heated filament (heating rates of 10³–10⁴ K s^?1) and laser ignition (heating rate ～10⁶ K s^?1) experiments. The developed heterogeneous reaction model predicts a sharp temperature increase, which can be associated with ignition when the laser power approaches the experimental ignition threshold. In experiments, particles ignited by the laser beam are observed to explode, indicating a substantial gas release accompanying ignition. For the heated filament experiments, the model predicts exothermic reactions at the temperatures, at which ignition is observed experimentally; however, strong thermal contact between the metal filament and powder prevents the model from predicting the thermal runaway. It is suggested that oxygen gas release from decomposing CuO, as observed from particles exploding upon ignition in the laser beam, disrupts the thermal contact of the powder and filament; this phenomenon must be included in the filament ignition model to enable prediction of the temperature runaway.     

Effect of UV irradiation on the structural,optical and electrical properties of platinum

Investigations are performed on thermal, optical and electrical response of UV laser-irradiated platinum (Pt). 4N pure, annealed and fine polished samples are exposed to the KrF Excimer laser (248 nm, 20 ns, 50 mJ) under vacuum ～10^?6 torr at different laser fluences (0.5–2.5 J/cm²). Space-resolved plasma plume dynamics is studied by analyzing the captured plume images with the help of a computer controlled image-grabbing system. The irradiated targets are characterized for surface morphology, structural, optical and electrical investigations using the diagnostics; scanning electron microscopy, X-ray diffraction, rotating compensator auto-aligned ellipsometer and four-point probe, respectively. The value of maximum intensity emitted by Pt plasma plume is 250 grey scales. Surfaces of the target metals are modified by craters, moltens and redeposited material. Laser-induced periodic surface structures are produced at low laser fluence. Irradiation of Pt causes changes in diffracted X-rays intensity and grain sizes, dislocation in line densities and strain in the target materials. Considerable changes occur in optical parameters as well. A decrease in electrical conductivity of the irradiated targets also takes place in an exponential way with the change in laser fluence.     

Nanosecond laser ablation for pulsed laser deposition of yttria

A thermal model to describe high-power nanosecond pulsed laser ablation of yttria (Y₂O₃) has been developed. This model simulates ablation of material occurring primarily through vaporization and also accounts for attenuation of the incident laser beam in the evolving vapor plume. Theoretical estimates of process features such as time evolution of target temperature distribution, melt depth and ablation rate and their dependence on laser parameters particularly for laser fluences in the range of 6 to 30 J/cm² are investigated. Calculated maximum surface temperatures when compared with the estimated critical temperature for yttria indicate absence of explosive boiling at typical laser fluxes of 10 to 30 J/cm². Material ejection in large fragments associated with explosive boiling of the target needs to be avoided when depositing thin films via the pulsed laser deposition (PLD) technique as it leads to coatings with high residual porosity and poor compaction restricting the protective quality of such corrosion-resistant yttria coatings. Our model calculations facilitate proper selection of laser parameters to be employed for deposition of PLD yttria corrosion-resistive coatings. Such coatings have been found to be highly effective in handling and containment of liquid uranium.     

Non-equilibrium plasma production by pulsed laser ablation of gold

A gold target has been irradiated with a Q-switched Nd:Yag laser having 1064?nm wavelength, 9?ns pulse width, 900?mJ maximum pulse energy and a maximum power density of the order of 10¹⁰?W/cm². The laser–target interaction produces a strong gold etching with production of a plasma in front of the target. The plasma contains neutrals and ions having a high charge state. Time-of-flight (TOF) measurements are presented for the analysis of the ion production and ion velocity. A cylindrical electrostatic deflection ion analyzer permits measurement of the yield of the emitted ions, their charge state and their ion energy distribution. Measurements indicate that the ion charge state reaches 6⁺ and 10⁺ at a laser fluence of 100?J/cm² and 160?J/cm², respectively. The maximum ion energy reaches about 2?keV and 8?keV at these low and high laser fluences, respectively. Experimental ion energy distributions are given as a function of the ion charge state. Obtained results indicate that electrical fields, produced in the plume, along the normal to the plane of the target surface, exist in the unstable plasma. The electrical fields induce ion acceleration away from the target with a final velocity dependent on the ion charge state. The ion velocity distributions follow a “shifted Maxwellian distribution”, which the authors have corrected for the Coulomb interactions occurring inside the plasma.     

Elucidation of the nature of active oxygen in the reaction of low-temperature oxidation of CO on single crystal surfaces platinum and palladium

The temperature-programmed reaction (TPR) method, high-resolution electron energy loss spectroscopy (HREELS), and molecular beam method were used to elucidate the role surface reconstruction, subsurface oxygen (O_subs), and CO_ads concentration play in the low-temperature oxidation of CO on the Pt(100), Pt(410), Pd(111), and Pd(110) surfaces. The possibility of the formation of so-called hot oxygen atoms, which arise at the surface at the instant of dissociation of O_2ads molecules and can react with CO_ads at low temperatures (～150 K) to form CO₂, was examined. It was revealed that, when present in high concentration, CO_ads initiates the phase transition of the Pt(100)-(hex) reconstructed surface into the (1 × 1) non-reconstructed one and blocks fourfold hollow sites of oxygen adsorption (Pt₄-O_ads), thereby initiating the formation of weakly bound oxygen (Pt₂-O_ads), active in CO oxidation. For the Pt(410), Pd(111), and Pd(110) surfaces, the reactivity of O_ads with respect to CO was demonstrated to be dependent on the surface coverage of CO_ads. The ¹⁸O_ads isotope label was used to determine the nature of active oxygen reacting with CO at ～150–200 K. It was examined why a CO_ads layer produces a strong effect on the reactivity of atomic oxygen. The experimental results were confirmed by theoretical calculations based on the minimization of the Gibbs energy of the adsorption layer. According to these calculations, the CO_ads layer causes a decrease in the apparent activation energy E _act of the reaction due to changes in the type of coordination and in the energy of binding of O_ads atoms to the surface.     

Dynamics and spectroscopy of the laser plume from solid targets

The dynamics and the spectral kinetic characteristics of the plume emerging in the vicinity of graphite targets, pressed pellets consisting of zirconium oxide powder stabilized with yttrium (YSZ) and yttrium-aluminum oxides with neodymium (YAO:Nd), and single-crystal YAG:Cr are studied. The targets are irradiated in air at room temperature using a repetitively pulsed CO₂ laser with a wavelength of 10.6 μm, a peak power of up to 9 kW, a pulse energy of 1.69 J, and a pulse duration of 330 μs at a level of 0.1. The plume propagates normally to the target surface at an angle of 45° relative to the laser radiation. The spectral kinetic characteristics of the plume luminescence are discretely measured along the entire length. It is demonstrated that the plumes of all targets (except for the single-crystal YAG:Cr) represent the flows of a weakly nonequilibrium gas plasma with a temperature of 10 kK (graphite) and 3.1–4.7 kK (YSZ and YAO:Nd pressed pellets). The plume size is determined by the peak power of the laser pulse. The luminescence of the two-atom radicals (C₂ in graphite; ZrO and YO in YSZ; and YO, AlO, and NdO in YAO:Nd) dominates in all of the plumes. A single radical (YO) and the spectral lines of atoms and atomic ions are observed in the YAG:Cr plume. A relatively high temperature of the graphite plume is maintained owing to the energy of the exothermic reaction involving the association of carbon atoms and the energy of the vibrationally excited molecules resulting from this reaction. Original Text ? Astro, Ltd., 2006.     

Double-pulse laser ablation applied to reactive PLD method for synthesis of carbon nitride film: A second laser shot delay

Carbon nitride films were deposited using ablation of graphite target by second harmonic radiation of Nd:YAG laser in nitrogen atmosphere. To produce high hardness films, the deposited particles should have sufficient kinetic energy to provide their efficient diffusion on a substrate surface for formation of crystal structure. However, a shock wave is arisen in ambient gas as a consequence of laser plasma explosive formation. This shock wave reflected from the substrate interacts with plume particles produced by the first laser pulse and decreases their kinetic energy. This results in decrease of film crystallinity. To improve film quality, two successive laser pulses was proposed to be used. At adjusting time delay, the particles induced by the second pulse wilt serve as a piston, which will push forward both stopped particles ablated by the first pulse and arisen from chemical reactions in ambient gas. An X-ray photoelectron spectroscopy (XPS) analysis of deposited films has shown an increase of content of sp ³ carbon atoms corresponding to crystalline phase, if double-pulse configuration is employed. The luminescence of excited C₂ and CN molecules in laser plume at different distances from the target was studied to optimize the delay between laser pulses.     

Cathodoluminescence of thorium in the presence of O2, CO and gas mixtures of CO-O2 and CO-H2

The cathodoluminescence (2–6 keV incident electrons) observed from thorium (111) and (533) crystal faces was recorded and analyzed for surfaces produced under various conditions. The blue luminescence observed in the presence of a partial oxygen pressure ～ 133 μPa (～10^-6 Torr) was found to consist of a broad asymmetric major band that peaked around 468 nm on which weak bands or lines were superimposed at approximately 433, 489, 502, and 534 nm. The emission was almost totally extinguished in the presence of a partial CO pressure ～ 133 μPa (～10^-6 Torr). The thorium-oxygen cathodoluminescence (CL) is interpreted as arising from the formation of ThO₂ and the excitation of luminescence centers by the incident electron beam and their subsequent decay. The major luminescence at 468 nm arises from F centers in ThO₂. The weak bands at 433 and 534 nm may arise from surface F⁺ and F centers designated as F⁺_s and F_s. The former may also be due to an OH luminescence center. The two longer wavelength lines (489, 502 nm) superimposed on the broad major band at approximately 468 nm are interpreted as arising from Pr³⁺ impurities in the thorium lattice that gave rise to fluorescence emission. The line at 468 nm also may be due in part to the fluorescence of ThO. The cathodoluminescence spectra observed in the presence of CO, and (CO+O₂) and (CO+H₂) gas mixtures were consistent with an interpretation that O₂ in the gas phase was required in order to obtain ThO₂ on and below the surface to produce significant luminescence. Auger spectroscopy showed that exposure to CO left approximately as much oxygen on the surface as in the case of O₂ but did not produce appreciable cathodoluminescence.     

Generation of a fast-ion beam upon the interaction of a multiterawatt picosecond laser pulse with a solid target

The parameters of fast particles generated upon the interaction of 10¹⁹ W/cm² laser pulses with solid targets are studied. The spatial and energy parameters of fast ions are investigated. It is found that approximately 1–3% of the laser energy is transformed to the energy of mega-and submegaelectronvolt ions at laser pulse intensities ≥10¹⁸ W/cm². It is shown experimentally that an ion beam is directed perpendicular to the target surface. The analytic and numerical simulations agree with experimental results and predict the propagation of fast electrons in the mirror direction with respect to the incident laser beam and of ions perpendicular to the target. The theoretical calculations are compared with the experimental output and spectra of fast electrons and ions.     

Propagation of LaMnO3 laser ablation plume in oxygen gas

The propagation of LaMnO₃ laser ablation plume in oxygen background has been investigated using fast photography of overall visible plume emission and time-resolved optical emission spectroscopy. The plume expansion was studied with ambient oxygen pressures ranging from vacuum level to 100 Pa. Free-expansion, splitting, sharpening and stopping of the plume were observed at different pressures and time delays after the laser pulse. Time-resolved optical emission spectroscopy showed that oxides are mainly formed through reaction of the atomic species ablated from the target with oxygen in the gas-phase. These reactions mainly affect the content of lanthanum oxide in the plume, while emission of manganese oxide is barely observed in all the range of pressure investigated.     

Non-contact acoustic tests based on nanosecond laser ablation: Generation of a pulse sound source with a small amplitude

A method to generate a pulse sound source for acoustic tests based on nanosecond laser ablation with a plasma plume is discussed. Irradiating a solid surface with a laser beam expands a high-temperature plasma plume composed of free electrons, ionized atoms, etc. at a high velocity throughout ambient air. The shockwave generated by the plasma plume becomes the pulse sound source. A laser ablation sound source has two features. Because laser ablation is induced when the laser fluence reaches 10¹²–10¹⁴ W/m², which is less than that for laser-induced breakdown (10¹⁵ W/m²), laser ablation can generate a lower sound pressure, and the sound source has a hemispherical radiation pattern on the surface where laser ablation is generated. Additionally, another feature is that laser-induced breakdown sound sources can fluctuate, whereas laser ablation sound sources do not because laser ablation is produced at a laser beam–irradiation point. We validate this laser ablation method for acoustic tests by comparing the measured and theoretical resonant frequencies of an impedance tube.     

Collective behavior of laser-produced plasma from a multicomponent YBa2Cu3O7 target in air

2 Cu₃O₇, using a Q-switched Nd:YAG laser is investigated by time-resolved emission-spectroscopic techniques at various laser irradiances. It is observed that beyond a laser irradiance of 2.6×10¹¹ W cm^-2, the ejected plume collectively drifts away from the target with a sharp increase in velocity to 1.25×10⁶ cm s^-1, which is twice its velocity observed at lower laser irradiances. This sudden drift apparently occurs as a result of the formation of a charged double layer at the external plume boundary. This diffusion is collective, that is, the electrons and ions inside the plume diffuse together simultaneously and hence it is similar to the ambipolar diffusion of charged particles in a discharge plasma. Received: 30 January 1998/Revised version: 12 June 1998     

Emission of excited copper atoms in laser-produced erosion plasmas

The distribution of emission from excited states of a copper atom in erosion plasmas formed in vacuum by the action of neodymium laser pulses with a power density of (3–5)×10⁸ W/cm² on a copper target is studied. Averaged spectra and oscillograms of emission of Cu I lines were recorded in a region of 210–600 nm. Resonant lines of Cu I, lines of cascade transitions to resonant levels of Cu I, and lines from shifted levels of a copper atom are shown to possess the highest intensity. Oscillograms of emission at Cu I transitions have two peaks, which may be associated with two phases of surface evaporation of copper: under the action of a Nd³⁺:YAG laser pulse and radiation of the core of an erosion plasma plume. The relationship between the intensities of peaks in oscillograms of emission of Cu I lines points to the presence of a considerable cascade contribution to the population of the resonant states of Cu I and self-absorption of resonant lines of a copper atom at the first stage of evaporation of a copper target.     

Experimental investigation of plume expansion dynamics of nanosecond laser ablated Al with small incident angle

Experimental study of expansion dynamics of pulsed-laser ablation plasmas from Al is presented. A systematic investigation of plasma plume expansion is done. The laser beam is focused on the target with an incident angle between 0° and 20°. The results show that the plume growth is almost normal to the target surface, irrespective of the incident angle of the laser. Besides, the time evolution of the plasma plume geometry ratio at different incident angles shows that the incident angle of laser beam influences very slightly its shape at later delay time. The results imply that when the incident angle is small (ranging from 0° to 20°), the influence of the incident angle on the plume expansion is rather trivial.     

The absorption of incident beams during laser drilling of metals

Laser produced plasma plays an important role in the laser drilling of sheet metals as it can partially block and absorb the incident laser beam. A previous study of the transient properties of charged particles in the plasma plume has shown that, at low electron densities with high electron temperatures, laser drilling improves. This suggests that measurement of the absorption of the plasma plume is essential.The present study covers measurement of the absorption of a HeNe beam passing transversely through the plasma plume. The measurement was carried out using two fast response photodiodes and was repeated for sub-atmospheric pressures of air.The results obtained show that drilling is best at a pressure of 200 torr (2.7 x 10⁴ Pa) and rapid expansion of the flares is favourable at 2 mm above the surface. Coupling of absorption and heating is also best at this pressure.     

Computational and experimental study of the cluster size distribution in MAPLE

A combined experimental and computational study is performed to investigate the origin and characteristics of the surface features observed in SEM images of thin polymer films deposited in matrix-assisted pulsed laser evaporation (MAPLE). Analysis of high-resolution SEM images of surface morphologies of the films deposited at different fluences reveals that the mass distributions of the surface features can be well described by a power-law, Y(N) ∝ N^−t, with exponent −t ≈ −1.6. Molecular dynamic simulations of the MAPLE process predict a similar size distribution for large clusters observed in the ablation plume. A weak dependence of the cluster size distributions on fluence and target composition suggests that the power-law cluster size distribution may be a general characteristic of the ablation plume generated as a result of an explosive decomposition of a target region overheated above the limit of its thermodynamic stability. Based on the simulation results, we suggest that the ejection of large matrix-polymer clusters, followed by evaporation of the volatile matrix, is responsible for the formation of the surface features observed in the polymer films deposited in MAPLE experiments.     

Modulational instability of a laser beam in a longitudinal magnetized piezoelectric semiconductor

Using the hydrodynamic model of a homogeneous infinite plasma, the modulational instability of a laser beam with an acoustic and a helicon wave has been investigated in a piezoelectric semiconductor. The threshold electric field amplitude and the growth rate of the unstable mode have been obtained analytically and for n-InSb at 77 K the unstable mode is found to be propagating with a growth rate ≈10⁵ s^-1 when the crystal is irradiated with a 337 μm HCN laser.