Mechanisms of ablation-rate decrease in multiple-pulse laser ablation

We present two sets of experimental results on the ablation-rate decrease with increase of the number of consecutive laser pulses hitting the same spot on the target surface. We have studied laser ablation of a carbon target with nanosecond pulses in two different interaction regimes: one with a XeCl laser (λ=308 nm) and the other with a Nd:YAG laser (λ=1064 nm), in both cases at the intensity ∼5×10⁸ W/cm² Two different mechanisms were found to be responsible for the ablation-rate decrease; they are directly related to the two different laser–matter interaction regimes. The UV-laser interaction is in the regime of transparent vapour (surface absorption). The increase of the neutral vapour density in the crater produced by the preceding laser pulses is the main reason for the decrease of ablation rate. With the IR laser each single laser pulse interacts with a partially ionised plume. With increase of the number of pulses hitting the same spot on the target surface, the laser–matter interaction regime gradually changes from the near-surface absorption to the volume absorption, resulting in the decrease in absorption in the target and thus in the decrease in the ablation rate. The change in the evaporation rate was considered for both vacuum and reactive-gas environments. Received: 21 February 2001 / Accepted: 26 February 2001 / Published online: 23 May 2001     

Propagation regimes of intense circularly polarized laser beam in magnetoactive plasma

This paper presents an analytical and numerical investigation of an intense circularly polarized wave propagating along the static magnetic field parallel to oscillating magnetic field in magnetoactive plasma. In the relativistic regime such a magnetic field is created by pulse itself. The authors have studied different regimes of propagation with relativistic electron mass effect for magnetized plasma. An appropriate expression for dielectric tensor in relativistic magnetoactive plasma has been evaluated under paraxial theory. Two modes of propagation as extraordinary and ordinary exist; because of the relativistic effect, ultra-strong magnetic fields are generated which significantly influence the propagation of laser beam in plasma. The nature of propagation is characterized through the critical-divider curves in the normalized beam width with power plane For given values of normalized density (ω_p/ω) and magnetic field (ω_c/ω) the regions are namely steady divergence (SD), oscillatory divergence (OD) and self-focusing (SF). Numerical computations are performed for typical parameters of relativistic laser-plasma interaction: magnetic field B = 10-100 MG; intensity I = 10¹⁶ to 10²⁰ W/cm²; laser frequency ω = 1.1 × 10¹⁵ s⁻¹; cyclotron frequency ω_c = 1.7 × 10¹³ s⁻¹; electron density n_e = 2.18 × 10²⁰ cm⁻³. From the calculations, we confirm that a circularly polarized wave can propagate in different regimes for both the modes, and explicitly indicating enhancement in wave propagation, beam focusing/self-guiding and penetration of E-mode in presence of magnetic field.     

Laser impulse coupling at 130 fs

We measured the momentum coupling coefficient C_m and laser-generated ion drift velocity and temperature in the femtosecond (fs) region, over a laser intensity range from ablation threshold to about one hundred times threshold. Targets were several pure metals and three organic compounds. The organic compounds were exothermic polymers specifically developed for the micro-laser plasma thruster, and two of these used “tuned absorbers” rather than carbon particles for laser absorption. The metals ranged from Li to W in atomic weight. We measured time of flight (TOF) profiles for ions. Specific impulse reached record values for this type of measurement and ablation efficiency was near 100%. These measurements extend the laser pulsewidth three orders of magnitude downward in pulsewidth relative to previous reports. Over this range, we found C_m to be essentially constant. Ion velocity ranged from 60 to 180 km/s.     

Langmuir probe investigation of surface contamination effects on metals during femtosecond laser ablation

Characterisation of the plasma plume induced by femtosecond laser-metal interactions has been carried out using a Langmuir probe. A double peak distribution of ablated ions and electrons has been recorded during time of flight (TOF) experiments for three metals studied (Ag, Cu and Ni). The first peak which occurs earliest in time is attributed to a surface layer of contaminants on the metal surface as it is shown to disappear after several laser shots. The re-growth of this peak, thought to be due to a recontamination process on the surface of the metal, is the subject of this paper. Two re-contamination mechanisms were considered; adsorption of contaminants from the ambient gas, and surface diffusion effects from the surrounding contaminants. Re-contamination rates for Ag, Cu and Ni were studied under two distinct gas pressures to investigate the contamination effects from the ambient. Effects arising from surface diffusion were investigated by raising the temperature of the metal sample to increase the surface mobility of the contaminants. The total contribution of contamination species present in the ablation plume was estimated by conducting angular distribution measurements of the plume. Surface diffusion of the surrounding contaminants was found to be the dominant recontamination process.     

Numerical study of ultra-short laser ablation of metals and of laser plume dynamics

Numerical modeling is used to investigate the physical mechanisms of the interaction of ultra-short (sub-picosecond) laser pulses with metallic targets. The laser–target interaction is modeled by using a one-dimensional hydrodynamic code that includes the absorption of laser radiation, the electronic heat conduction, the electron-phonon or electron–ion energy exchange, as well as a realistic equation of state. Laser fluences typical for micromachining are considered. The results of the 1D modeling are then used as the initial conditions for a 2D plasma expansion model. The dynamics of laser plume expansion in femtosecond regime is investigated. Calculations show that the plasma plume is strongly forward directed. In addition, a two-peaked axial density profile is obtained for 400 nm laser wavelength. The calculation results agree with the experimental observations. PACS 52.38.Mf; 02.60.Cb     

Emission spectroscopy of laser ablation plume: Composition analysis of a target in water

Emission spectra of the laser ablation plume formed by the irradiation of Cu65/Zn35 binary alloy in water at the room temperature with 150-ns pulsed laser were measured. The spectra were analyzed by comparing with the theoretical calculation based on the assumption that self-absorption effect is negligible and that the same temperature can be applied to Cu atoms and Zn atoms in the plume. The calculation reproduced the spectra very well and gave reasonable temperature as a best-fit parameter. However, the best-fit value of the Cu atomic density relative to Zn is significantly low compared with the target composition. Care should be taken to perform in situ LIBS in liquid due to the complicated plume formation mechanism and dynamics of material intake into the plume.     

Enhanced cleaning of photoresist film on a transparent substrate by backward irradiation of a Nd:YAG laser

Laser cleaning of a photoresist (PR) on a glass substrate using ns-pulsed Nd:YAG laser was studied. The direction of the substrate facing the laser beam was varied as a main parameter as well as the power of the laser beam. The backward irradiation (BWI) of the third harmonic beam (355 nm) completely removed 1.2 μm thick PR layer with three pulses at 1.5 J/cm² leaving no residues behind; while the forward irradiation (FWI) at the same condition just partially cleaned it. To investigate the difference of removal mechanisms between irradiation directions, the size distributions of particulates generated during laser cleaning were observed using an optical particle counter. The concentration of micron-sized particulates increased with increasing laser fluence up to 1 J/cm² for FWI and 0.5 J/cm² for BWI and then decreased at higher fluences because the target was a very thin film. The concentration of larger particulates for BWI was much higher than that for FWI implying the difference in removal mechanisms. In consideration of the size characteristics of the particulates and the temperature profiles of the PR layer, the most probable distinct mechanism for the BWI would be a blasting due to high temperature at the PR/glass interface. The particulate number concentration decreased rapidly after the completion of cleaning, suggesting that the measurement of the particulate concentration could detect the progress of the cleaning. Our results demonstrated that the backward irradiation will be useful for the laser cleaning of film-type contaminants on an optically transparent substrate.     

Absorption and saturation mechanisms in aluminium laser ablated plasmas

-2 ). The interpretation of the ion TOF distributions in terms of theoretical shifted Maxwell–Boltzmann distributions produces a good agreement with the experimental data. This has allowed us to infer the ion flow velocity and temperature associated with the measured TOF distributions, as well as the ion kinetic energies as a function of the laser fluence. We have also studied the total ion yield at different laser fluences. Our results show that all the plume parameters investigated are increasing functions of the laser fluence until a saturation plateau is reached at high fluences (>20 Jcm^-2). We ascribe this saturation behav iour to strong absorption and partial, or total, reflection of the laser light by the hot plasma produced by the leading edge of the intense laser pulse. This interpretation is supported by a semi-quantitative analysis of the laser photon absorption and ionization mechanisms in Al plasma, at both laser wavelengths. Received: 6 January 1997/Accepted: 14 March 1997     

Synthesis of nanoclusters by nanosecond laser ablation: Direct simulation Monte Carlo modelling

Collisional processes leading to the formation of nanoparticles in a laser-ablated plume are numerically simulated with the aid of an atomistic-level model based on direct simulation Monte Carlo (DSMC) method. The formation of nanoparticles in nanosecond laser ablation of a mono-atomic target is investigated in the presence of an inert background gas. The DSMC procedure is modified in order to account for numerous plume species and to describe several reactions (i.e., recombination/dissociation, sticking, evaporation) taking place in the plume and affecting the size and spatial distribution of the produced nanoclusters. Calculation results allow us to visualize the nanoparticles and to correlate their space distributions with plume dynamics. In addition, cluster size distributions are investigated at different pressures. The effects of the background gas on cluster formation within the plume are furthermore shown.     

Effect of focusing geometry on the continuous optical discharge properties

We studied the effect of the laser beam focusing geometry on the continuous optical discharge (COD) properties. We used a full two-dimensional radiative gas-dynamic model for the COD, maintained by a vertical CO₂ laser beam in free air atmosphere, in the Earth's gravitational field. The model takes into account all of the factors that are of importance in laser-sustained plasma processes, and uses realistic quasi optics to describe the laser radiation propagation. Results are presented for the optical discharge parameters as functions of applied laser power and degree (f-number) to which the laser beam is focused.     

Studies of craters’ dimension for long-pulse laser ablation of metal targets at various experimental conditions

Long pulse laser shots of the PALS iodine laser in Prague have been used to obtain metal target ablation at various experimental conditions. Attention is paid mainly to the dependencies of the crater diameter on the position of minimum laser-focus spot with regard to the target surface, by using different laser wavelengths and laser energies. Not only a single one, but two minima, independently of the wavelength, of the target irradiation angle and of the target material, were recorded. Significant asymmetries, ascribed to the non-linear effects of intense laser beam with pre-formed plasma, were found, too. Estimations of ejected mass per laser pulse are reported and used to calculate the efficiency of laser-driven loading. Results on metal target ablation and crater formation at high intensities (from 2 × 10¹³ to 3 × 10¹⁶ W/cm²) are presented and compared. Crater depth, crater diameter and etching yield are reported versus the laser energy, in order to evaluate the ablation threshold fluence.     

Fundamentals and applications of polymers designed for laser ablation

The ablation characteristics of various polymers were studied at low and high fluences for an irradiation wavelength of 308 nm. The polymers can be divided into three groups, i.e. polymers containing triazene groups, designed ester groups, and reference polymers, such as polyimide. The polymers containing the photochemically most active group (triazene) exhibit the lowest thresholds of ablation (as low as 25 mJ cm^-2) and the highest etch rates (e.g. 250 nm/pulse at 100 mJ cm^-2), followed by the designed polyesters and then polyimide. Neither the linear nor the effective absorption coefficients have a clear influence on the ablation characteristics. The different behavior of polyimide might be explained by a pronounced thermal part in the ablation mechanism. The laser-induced decomposition of the designed polymers was studied by nanosecond interferometry and shadowgraphy. The etching of the triazene polymer starts and ends with the laser pulse, indicating photochemical ablation. Shadowgraphy reveals mainly gaseous products and a pronounced shockwave in air. The designed polymers were tested for an application as the polymer fuel in laser plasma thrusters. Received: 21 October 2002 / Accepted: 20 January 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +41-56/3104-412, E-mail: thomas.lippert@psi.ch     

Self-focusing of Gaussian laser beam in collisionless plasma and its effect on stimulated Raman scattering process

This paper presents an investigation of self-focusing of Gaussian laser beam in collisionless plasma and its effect on stimulated Raman scattering process. The pump beam interacts with a pre-excited electron plasma wave thereby generating a back-scattered wave. On account of Gaussian intensity distribution of laser beam, the time independent component of the ponderomotive force along a direction perpendicular to the beam propagation becomes finite, which modifies the background plasma density profile in a direction transverse to pump beam axis. This modification in density affects the incident laser beam, electron plasma wave and back-scattered beam. We have set up the non-linear differential equations for the beam width parameters of the main beam, electron plasma wave, back-scattered wave and SRS-reflectivity by taking full non-linear part of the dielectric constant of collisionless plasma with the help of moment theory approach. It is observed from the analysis that focusing of waves greatly enhances the SRS reflectivity.     

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.     

Comparison of two theories during self-focusing of Gaussian laser beam in thermal conduction-loss predominant plasmas

In the present paper, self-focusing phenomenon occurring as a result of non-linear interaction of intense laser beam with thermal conduction-loss predominant plasmas is studied by following both approaches viz. paraxial theory approach and moment theory approach. Non-linear differential equations for the beam width parameters of laser beam have been set up and solved numerically in both cases to study the variation of beam width parameters with normalized distance of propagation. Effects of laser intensity as well as plasma density on the beam width parameters have also been analyzed. It is observed from the analysis that in case of moment theory approach, strong self-focusing of laser beam is observed as compared to paraxial theory approach.     

Mechanisms of small clusters production by short and ultra-short laser ablation

The mechanisms involved into the formation of clusters by pulsed laser ablation are studied both numerically and experimentally. To facilitate the model validation by comparison with experimental results, the time and length scales of the simulation are considerably increased. This increase is achieved by using a combination of molecular dynamics (MD) and the direct simulation Monte Carlo (DSMC) methods. The combined MD-DSMC model is then used to compare the relative contribution of the two channels of the cluster production by laser ablation: (i) direct cluster ejection upon the laser-material interaction, and (ii) collisional sticking and aggregation in the ablated gas flow. Calculation results demonstrate that both of these mechanisms play a role. The initial cluster ejection provides cluster precursors thus eliminating the three-body collision bottleneck in the cluster growth process. The presence of clusters thus facilitates the following collisional condensation and evaporation processes. The rates of these processes become considerable, leading to the modification of not only the plume cluster composition, but also the dynamics of the plume expansion. Calculation results explain several recent experimental findings.     

Theoretical determination of the ablation rate of metals in multiple-nanosecond laser pulses irradiation regime

A detailed understanding of the physical determinants of the ablation rate in multiple nanosecond laser pulses regime is of key importance for technological applications such as patterning and pulsed-laser deposition. Here, theoretical modeling is employed to investigate the ablation of thick metallic plates by intense, multiple nanosecond laser pulses. A new photo-thermal model is proposed, in which the complex phenomena associated to the ablation process are accounted for as supplementary terms of the classical heat equation. The pulsed laser ablation in the nanosecond regime is considered as a competition between thermal vapourization and melt ejection under the action of the plasma recoil pressure. Computer simulations using the photo-thermal model presented here and the comparison of the theoretical results with experiment indicate two different mechanisms that contribute to the decrease of the ablation efficiency. First, during the ablation process the vapour/plasma plume expanding above the irradiated target attenuates the laser beam that reaches the sample, leading to a marked decrease of the ablation efficiency. Additional attenuation of the laser beam incident on the sample is produced due to the heating of the plasma by the absorption of the laser beam into the plasma plume. The second mechanism by which the ablation efficiency decreases consists of the reduction of the incident laser intensity with the lateral area, and of the melt ejection velocity with the depth of the hole.     

Laser-plasma interaction in the context of inertial fusion: experiments and modeling

Many nonlinear processes may affect the laser beam propagation and the laser energy deposition in the underdense plasma surrounding the pellet. These processes, associated with anomalous and nonlinear absorption mechanisms, are fundamental issues in the context of Inertial Confinement Fusion. The work presented in this article refers to laser-plasma interaction experiments which were conducted under well-controlled conditions, and to their theoretical and numerical modeling. Thanks to important diagnostics improvements, the plasma and laser parameters were sufficiently characterized in these experiments to make it possible to carry out numerical simulations modeling the laser plasma interaction in which the hydrodynamics conditions were very close to the experimental ones. Two sets of experiments were carried out with the LULI 2000 and the six beam LULI laser facilities. In the first series of experiments, the interaction between two single hot spots was studied as a function of their distance, intensity and light polarization. In the second series, the intensity distribution of stimulated Brillouin scattering (SBS) inside the plasma was studied by means of a new temporally resolved imaging system. Two-dimensional (2D) simulations were carried out with our code Harmony2D in order to model these experiments. For both series of experiments, the numerical results show a very good agreement with the experimental ones for what concerns the main SBS features, namely the spatial and temporal behavior of the SBS-driven acoustic waves, as well as the average SBS reflectivities. Thus, these well diagnosed experiments, carried out with well defined conditions, make it possible to benchmark our theoretical and numerical modelings and, hence, to improve our predictive capabilities for future experiments.