Modeling of UV pulsed-laser ablation of metallic targets

A model to describe the laser ablation of metallic targets is presented. It accounts for the main physical processes involved in the laser–solid–plasma interaction by considering the photon absorption and the ionization mechanisms that are active in the plasma, as well as the laser-produced plasma kinetics. The model is used to simulate the laser ablation of aluminum targets irradiated with a 6-ns UV laser pulse at 0.35 μm, and the results are compared with experimental findings. Calculations show that all the investigated plasma parameters strongly depend on the laser intensity until a roll-off is reached at irradiance ≥1.5 GW cm^-2. The satisfactorily good agreement between model predictions and experimental findings confirms that laser–plasma interaction processes and plasma kinetics play a relevant role during nanosecond laser ablation of metals in the laser intensity range of concern in this study. Received: 12 February 1999 / Accepted: 12 April 1999 / Published online: 7 July 1999     

Acoustic wave monitoring of the excimer laser ablation of YBCO high-Tc superconductor

Monitoring the amplitude and the delay of arrival of the pressure waves generated during the interaction of laser pulses with YBCO in air, we can determine the vaporization and the ablation thresholds, the etching rate, the change of the acoustic wave velocity and the effect of plasma shielding on the etching rate. The steep increase of the amplitude and the order-of-magnitude increase of the etching rate above the ablation threshold, suggest that the laser–target coupling mechanism changes from (thermal) vaporization below threshold to a rapid solid-to-gas phase transition. The dumping of the acoustic waves following the ablation with successive laser pulses correlates with the evolution of the YBCO high-T_c superconductor surface morphology, which is known to relate to the deposition rate and the surface morphology of pulsed-laser-deposited high-T_c thin films. Received: 7 January 2000 / Accepted: 9 October 2000 / Published online: 25 July 2001     

Crown-like structure development on titanium exposed to multipulse Nd:YAG laser irradiation

We report micrometre-sized crown-like structure growth on a Ti surface by multipulse Nd:YAG (λ=1.064 μm,τ=170 ns) laser irradiation in air at atmospheric pressure. The irradiation was performed at 8×10⁷ W/cm² laser-pulse intensity, below the ablation threshold. A ring-shape structure develops in the centre of the irradiation spot after the action of five laser pulses. The further increase of the laser-pulse number leads gradually to a crown-like structure, which has, for 150 pulses, a height of 120–140 μm above the non-irradiated Ti surface. The forming crater’s depth does not exceed the height of the grown structure. In the neighbouring zone, after the action of 25 laser pulses, microcracks of the oxide surface layer develop. With the next pulses this leads to the formation of a surface microrelief. The crown-like-structure growth is originated by molten material movement attributed to the laser-induced plasma-recoil pressure. Received: 6 June 2001 / Accepted: 6 January 2002 / Published online: 26 March 2002     

Characterization of excimer laser ablation generated pepsin particles using multi-wavelength photoacoustic instrument

Preparation of organic thin layers on various special substrates using the pulsed laser deposition (PLD) technique is an important task from the point of view of bioengineering and biosensor technologies. Earlier studies demonstrated that particle ejection starts during the ablating laser pulse resulting in significant shielding effects which can influence the real fluence on the target surface and consequently the efficiency of layer preparation. In this study, we introduce a photoacoustic absorption measurement technique for in-situ characterization of ablated particles during PLD experiments. A KrF excimer laser beam (λ=248 nm, FWHM=18 ns) was focused onto pepsin targets in a PLD chamber; the applied laser fluences were 440 and 660 mJ/cm². We determined the wavelength dependence of optical absorption and mass specific absorption coefficient of laser ablation generated pepsin aerosols in the UV–VIS–NIR range. On the basis of our measurements, we calculated the absorbance at the ablating laser wavelength, too. We demonstrated that when the laser ablation generated pepsin aerosols spread through the whole PLD chamber the effect of absorptivity is negligible for the subsequent pulses. However, the interaction of the laser pulse and the just formed particle cloud generated by the same pulse is more significant.     

Numerical modeling of laser–matter interaction in the region of “low” laser parameters

The interaction of laser radiation with matter leads to the certain kinds of modelling of its surface or volume. These effects have been demonstrated for a lot of materials, even causing the formation of new scientific and industrial domain, which is undoubtedly laser material processing and as well as laser cleaning of artworks. Those applications lie in the so-called “low' region of laser energy densities, represented for short laser pulses by power densities below 10⁹ W/cm². Paper presents set of equations describing in one-dimensional (1D) model phenomena accompanying to laser–matter interaction. Target geometry includes two and four layers of different materials, irradiated by ns laser pulses. Effects of radiation absorption and transport, heat conductivity, target transit to plastic state, melting and evaporation are taken into consideration. The part of the paper is devoted to the discussion of numerical results, selected in such a way to illustrate the phenomenon of radiation interaction with materials as well as to show, in whole, possibilities of computer simulation methods.     

Measurement of femtosecond laser-induced damage and ablation thresholds in dielectrics

The paper is focused on the importance of accurate determination of surface damage/ablation threshold of a dielectric material irradiated with femtosecond laser pulses. We show that different damage characterization techniques and data treatment procedures from a single experiment provide complementary physical results characterizing laser–matter interaction. We thus compare and discuss two regression techniques, well adapted to the measurement of laser ablation threshold, and a statistical approach giving the laser damage threshold and further information concerning the deterministic character of femtosecond damage. These two measurements are crucial for laser micromachining processes and high peak-power laser technology in general.     

Impact of the lasr wavelength and fluence on the ablation rate of aluminium

The dependence of the ablation rate of aluminium on the fluence of nanosecond laser pulses with wavelengths of 532 nm and respectively 1064 nm is investigated in atmospheric air. The fluence of the pulses is varied by changing the diameter of the irradiated area at the target surface, and the wavelength is varied by using the fundamental and the second harmonic of a Q-switched Nd-YAG laser system. The results indicate an approximately logarithmic increase of the ablation rate with the fluence for ablation rates smaller than ∼6 μm/pulse at 532 nm, and 0.3 μm/pulse at 1064 nm wavelength. The significantly smaller ablation rate at 1064 nm is due to the small optical absorptivity, the strong oxidation of the aluminium target, and to the strong attenuation of the pulses into the plasma plume at this wavelength. A jump of the ablation rate is observed at the fluence threshold value, which is ∼50 J/cm² for the second harmonic, and ∼15 J/cm² for the fundamental pulses. Further increasing the fluence leads to a steep increase of the ablation rate at both wavelengths, the increase of the ablation rate being approximately exponential in the case of visible pulses. The jump of the ablation rate at the threshold fluence value is due to the transition from a normal vaporization regime to a phase explosion regime, and to the change of the dimensionality of the hydrodynamics of the plasma-plume.      

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.     

Long duration light emission from femtosecond laser–target interactions

Time resolved emission from the interaction of ultra-short (∼200 fs) laser pulses with aluminum and copper targets was investigated. Measurements show that emission from the laser produced plasma in air is significantly more intense than in near vacuum conditions and that the emission in air can extend for periods exceeding 100 ns. Modeling the laser–target–air coupling shows that the laser–target interaction can lead to blast wave shock waves being launched in the ambient air and that the emission from the shocked air dominates over emission from the target surface. The long term emission measurements in air are in agreement with the modeling results.     

Ultra-fast laser absorption and ablation dynamics in wide-band-gap dielectrics

The highly nonlinear laser–matter interaction conditions produced by high-intensity amplified ultra-fast laser pulses have proven to be beneficial in the processing of normally transparent wide-band-gap dielectric materials. This article presents experimental studies of the ultra-fast laser absorption process in three wide-band-gap dielectrics: fused silica, calcium fluoride, and sapphire. Time-resolved measurements of the probe transmissivity and reflectivity show both the formation of dense free-electron plasma at the surface due to nonlinear absorption of the laser pulses and rapid structural damage on the order of a few picoseconds. Pump–probe data with intense pump and probe pulses was also correlated to atomic force microscopy measurements of the ablated volume. It was observed that the material removal peaked near zero delay between the pulses and decreased within a temporal separation of about 1 ps. PACS 52.38.Mf; 78.47.+p; 79.20.Ds     

Defect capture under rapid solidification of the melt induced by the action of femtosecond laser pulses and formation of periodic surface structures on a semiconductor surface

A theory of defect-strain instability with formation of periodic surface relief in semiconductors irradiated by ultra-short (τ_p=10^-13 s) powerful laser pulses is developed. The period and time of formation of surface relief are calculated. Regimes of multi-pulse laser ablation leading to formation of either a smooth surface or arrays of surface-relief spikes are pointed out and corresponding experimental results are interpreted from the viewpoint of the developed theory. Received: 4 December 2000 / Accepted: 23 July 2001 / Published online: 11 February 2002     

Model for laser-induced thermal degradation and ablation of polymers

Ablation of organic polymers is described on the basis of photothermal bond breaking within the bulk material. Here, we assume a first-order chemical reaction, which can be described by an Arrhenius law. Ablation starts when the density of broken bonds at the surface reaches a certain critical value. In order to understand the ablation behavior near the threshold fluence, φ_th, non-stationary regimes must be considered. The present treatment reveals several qualitative differences with respect to models that treat ablation as a surface process: (i) Ablation starts sharply with a front velocity that has its maximum value just after the onset. (ii) The transition to the quasi-stationary ablation regime is faster. (iii) Near threshold, the ablated depth h has a square-root dependence on laser fluence, i.e., h∝(φ-φ_th)^1/2. The ablation velocity is very high even near φ_th. (iv) With φ≈φ_th ablation starts well after the laser pulse. (v) The depletion of species is responsible for the Arrhenius tail observed with fluences φ≤φ_th. (vi) Residual modification of material has maximum near the threshold. (vii) Stationary regimes of ablation demonstrate change of effective activation energy with laser intensity. The model calculations are applied to Polyimide (Kapton^TM H). Here, differences in single-pulse ablated depth determined from mass loss and profilometry should be about 10 nm. Received: 16 February 1999 / Accepted: 18 February 1999 / Published online: 28 April 1999     

Laser-induced plasma-assisted ablation of fused quartz using the fourth harmonic of a Nd+:YAG laser

+ :YAG laser (266 nm) is reported. With the assistance of plasma resulting from laser irradiation on a metal target, the fused-quartz substrate is easily etched by the 266-nm laser beam in spite of the fact that the substrate is transparent to this wavelength. In contrast, no ablation takes place without the metal target, but damage is generated on the substrate surface. The ablated region is observed by optical microscopy and scanning probe microscopy (SPM), which reveal a fine grating structure (line spacing of 20 μm) without any severe damage. A series of experiments on the dependence of the ablation rate and the threshold laser fluence on ablation parameters, such as laser fluence, the number of pulses, and the distance between the fused quartz and the metal target is performed. On the basis of the results, three possible mechanisms of direct plasma interaction, plasma heating, and metal film deposition are discussed. Received: 27 February 1998/Accepted: 5 June 1998     

Femtosecond pulsed laser ablation of thin gold film

Laser micromachining on 1000 nm-thick gold film using femtosecond laser has been studied. The laser pulses that are used for this study are 400 nm in central wavelength, 150 fs in pulse duration, and the repetition rate is 1 kHz. Plano-concave lens with a focal length of 19 mm focuses the laser beam into a spot of 3 μm (1/e² diameter). The sample was translated at a linear speed of 400 μm/s during machining. Grooves were cut on gold thin film with laser pulses of various energies. The ablation depths were measured and plotted. There are two ablation regimes. In the first regime, the cutting is very shallow and the edges are free of molten material. While in the second regime, molten material appears and the cutting edges are contaminated. The results suggest that clean and precise microstructuring can be achieved with femtosecond pulsed laser by controlling the pulse energy in the first ablation regime.     

Identification of non-thermal and thermal processes in femtosecond laser-ablated aluminum

Non-thermal and thermal processes due to femtosecond laser ablation of aluminum (Al) at low, moderate, and high-fluence regimes are identified by Atomic Force Microscope (AFM) surface topography investigations. For this purpose, surface modifications of Al by employing 25 fs Ti: sapphire laser pulses at the central wavelength of 800 nm have been performed to explore different nano- and microscale features such as hillocks, bumps, pores, and craters. The mechanism for the formation of these diverse kinds of structures is discussed in the scenario of three ablation regimes. Ultrafast electronic and non-thermal processes are dominant in the lower fluence regime, whereas slow thermal processes are dominant at the higher fluence regime. Therefore, by starting from the ablation threshold three different fluence regimes have been chosen: a lower fluence regime (0.06–0.5 J cm^?2 single-shot irradiation under ultrahigh vacuum condition and 0.25–2.5 J cm^?2 single-shot irradiation in ambient condition), a moderate-fluence regime (0.25–1.5 J cm^?2 multiple-shot irradiation), and a high-fluence regime 2.5–3.5 J cm^?2 multiple-shot irradiation. For the lower fluence (gentle ablation) regime, around the ablation threshold, the unique appearance of individual, localized Nano hillocks typically a few nanometers in height and less than 100 nm in diameter are identified. These Nano hillock-like features can be regarded as a nonthermal, electronically induced phase transition process due to localized energy deposition as a result of Coulomb explosion or field ion emission by surface optical rectification. At a moderate-fluence regime, slightly higher than ablation threshold multiple-pulse irradiation produces bump-formation and is attributed to ultrafast melting (plasma formation). The high-fluence regime results in greater rates of material removal with highly disturbed and chaotic surface of Al with an appearance of larger protrusions at laser fluence well above the ablation threshold. These nonsymmetrical shapes due to inhomogeneous nucleation, cluster formation, and resolidification of a metallic surface after melting are attributable to slow thermal processes (ps time scale).     

Surface wettability of silicon substrates enhanced by laser ablation

Laser–ablation techniques have been widely applied for removing material from a solid surface using a laser–beam irradiating apparatus. This paper presents a surface–texturing technique to create rough patterns on a silicon substrate using a pulsed Nd:YAG laser system. The different degrees of microstructure and surface roughness were adjusted by the laser fluence and laser pulse duration. A scanning electron microscope (SEM) and a 3D confocal laser–scanning microscope are used to measure the surface micrograph and roughness of the patterns, respectively. The contact angle variations between droplets on the textured surface were measured using an FTA 188 video contact angle analyzer. The results indicate that increasing the values of laser fluence and laser pulse duration pushes more molten slag piled around these patterns to create micro-sized craters and leads to an increase in the crater height and surface roughness. A typical example of a droplet on a laser–textured surface shows that the droplet spreads very quickly and almost disappears within 0.5167 s, compared to a contact angle of 47.9° on an untextured surface. This processing technique can also be applied to fabricating Si solar panels to increase the absorption efficiency of light.     

Cumulative and continuous laser vaporization synthesis of single wall carbon nanotubes and nanohorns

The conditions for the scaled synthesis of single wall carbon nanotubes (SWNTs) and single wall carbon nanohorns (SWNHs) by laser vaporization at high temperatures are investigated and compared using in situ diagnostics. An industrial Nd:YAG laser (600 W, 1–500 Hz repetition rate) with tunable pulse widths (0.5–50 ms) is utilized to explore conditions for high-yield production. High-speed videography (50000 frames/s) of the laser plume and pyrometry of the target surface are correlated with ex situ high resolution transmission electron microscopy analysis of the products for pure carbon targets and carbon/catalyst targets to understand the effects of the processing conditions on the resulting nanostructures. Carbon is shown to self-assemble into single-wall nanohorn structures at rates of ∼1 nm/ms, which is comparable to the catalyst-assisted SWNT growth rates. Two regimes of laser ablation, cumulative ablation by multiple pulses and continuous ablation by individual pulses, were explored. Cumulative ablation with spatially overlapping 0.5-ms pulses is favorable for the high yield and production rate of SWNTs at ∼6 g/h while continuous ablation by individual long laser pulses (∼20 ms) at high temperatures results in the highest yield of SWNHs at ∼10 g/h. Adjustment of the laser pulse width is shown to control SWNH morphology.     

Drilling rate of five metals with picosecond laser pulses at 355, 532, and 1064 nm

Experimental results on picosecond laser processing of aluminum, nickel, stainless steel, molybdenum, and tungsten are described. Hole drilling is employed for comparative analysis of processing rates in an air environment. Drilling rates are measured over a wide range of laser fluences (0.05–20?J/cm²). Experiments with picosecond pulses at 355?nm are carried out for all five metals and in addition at 532?nm, and 1064?nm for nickel. A comparison of drilling rate with 6-ps and 6-ns pulses at 355?nm is performed. The dependence of drilling rate on laser fluence measured with picosecond pulses demonstrates two logarithmic regimes for all five metals. To determine the transition from one regime to another, a critical fluence is measured and correlated with the thermal properties of the metals. The logarithmic regime at high-fluence range with UV picosecond pulses is reported for the first time. The energy efficiency of material removal for the different regimes is evaluated. The results demonstrate that UV picosecond pulses can provide comparable quality and higher processing rate compared with literature data on ablation with near-IR femtosecond lasers. A significant contribution of two-photon absorption to the ablation process is suggested to explain high processing rate with powerful UV picosecond pulses.     

Femtosecond ablation of ultrahard materials

Several ultrahard materials and coatings of definite interest for tribological applications were tested with respect to their response when irradiated with fs laser pulses. Results on cemented tungsten carbide and on titanium carbonitride are reported for the first time and compared with outcomes of investigations on diamond and titanium nitride. The experiments were carried out in air, in a regime of 5–8 J/cm² fluences, using the beam of a commercial Ti:sapphire laser. The changes induced in the surface morphology were analysed with a Nomarski optical microscope, and with SEM and AFM techniques. From the experimental data and from the calculated incident energy density distributions, the damage and ablation threshold values were determined. As expected, the diamond showed the highest threshold, while the cemented tungsten carbide exhibited typical values for metallic surfaces. The ablation rates determined (under the above-mentioned experimental conditions) were in the range 0.1–0.2 μm per pulse for all the materials investigated. Received: 31 August 2001 / Accepted: 3 December 2001 / Published online: 20 March 2002     

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