Controlling energy coupling and particle ejection from aluminum surfaces irradiated with ultrashort laser pulses

Hydrodynamic simulations are used to evaluate the potential of ultrashort laser pulses to localize energy at metallic surfaces, in our case aluminum. The emphasis is put on the dynamic sequence of laser energy deposition steps during the electron-ion nonequilibrium stage and the subsequent matter transformation phases. The simulations indicate correlated optical and thermodynamical states associated to specific electronic collisional mechanisms. The timescales of energy deposition deliver a guideline for using relevant relaxation times to improve the energy coupling into the material. We focus on a class of pump-probe experiments which investigate energy storage and particle emission from solids under ultrafast laser irradiation. Moreover, we have used our model to explain the experimentally observed optimization of energy coupling by tailoring temporal laser intensity envelopes and its subsequent influence on the ablation rate and on the composition of ablation products. Potential control for nanoparticle generation is discussed.     

Vaporization and Plasma Shielding during High Power Nanosecond Laser Ablation of Silicon and Nickel

A thermal model to describe the high-power nanosecond pulsed laser ablation is presented. It involves the vaporization and the following plasma shielding effect on the whole ablation process. As an example of Si target, we obtainthe time evolution of the calculated surface temperature, ablation rate and ablation depth. It can be seen that plasma shielding plays a more important role in the ablation process with time. At the same time, the ablation depth with laser fluence based on different models is shown. Moreover, we simulate the pulsed laser irradiation Ni target. The evolution of the transmitted intensity and the variation of ablation depth per pulse with laser fluence are performed. Under the same experimental conditions, the numerical results calculated with our thermal model are more in agreement with the experimental data.     

Multi-material two-temperature model for simulation of ultra-short laser ablation

We investigate the interaction of 100 fs laser pulses with metal targets at moderate intensities (10¹² to 5 × 10¹³ W/cm²). To take into account effects of laser energy absorption and relaxation we develop a multi-material two-temperature model based on a combination of different approaches. The backbone of the numerical model is a high-order multi-material Godunov method in a purely Eulerian form. This formulation includes an interface-tracking algorithm and treats spallation at high strain rates and negative pressures. The model consistently describes the hydrodynamic motion of a two-temperature plasma and accounts for laser energy absorption, electron-phonon/ions coupling and electron heat conductivity. In particular, phase transitions are accurately taken into account by means of a wide-range two-temperature multi-phase equation of state in a tabular form. The dynamics of the phase transitions and the evolution of the heat-affected zone are modeled and analyzed. We have found that a careful treatment of the transport coefficients, as well as consideration of phase transitions is of a great importance in obtaining reliable numerical results. Calculation results are furthermore compared for two metals with different electron-phonon coupling parameters (Au and Al). We have found that the main part of ablated material results from fragmentation of melted phase caused by tensile stresses. A homogeneous nucleation mechanism alone does not explain experimentally observed ablation depth.     

Fundamentals and advantages of ultrafast micro-structuring of transparent materials

Experimental investigations using femtosecond and picosecond laser pulses at 800 nm illuminate the distinctions between the dynamics and nature of ultrafast processing of dielectrics compared with semiconductors and metals. Dielectric materials are strongly charged at the surface on the sub-ps time scale and undergo an impulsive Coulomb explosion prior to thermal ablation. Provided the laser pulse width remains in the ps or sub-ps time domain, this effect can be exploited for processing. In the case of thermal ablation alone, the high localization of energy accompanied by ultrafast laser micro-structuring is of great advantage also for high quality processing of thin metallic or semiconducting layers, in which the surface charge is effectively quenched. Received: 17 January 2003 / Accepted: 8 February 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +49-30/670-53-500, E-mail: d.ashkenasi@lmtb.dt RID="**" ID="**"Present address: LMTB GmbH, Berlin, Fabeckstr. 60–62, D-14195 Berlin, Germany     

Nanosecond and femtosecond UV laser ablation of polymers: Influence of molecular weight

We examine the nanosecond and femtosecond UV laser ablation of poly(methyl methacrylate) (PMMA) as a function of molecular weight (M_w). For laser ablation with nanosecond laser pulses, at the excimer wavelengths 248 nm and 193 nm, we show that high temperatures develop; yet the dynamics of material ejection differs depending on polymer M_w. The results on the nanosecond ablation of polymers are accounted within the framework of bulk photothermal model and the results of molecular dynamics simulations. Turning next to the 248 nm ablation with 500 fs laser pulses, the ablation threshold and etching rates are also found to be dependent on polymer M_w. In addition, ablation results in morphological changes of the remaining substrate. Plausible mechanisms are advanced.     

Minimization of cavitation effects in pulsed laser ablation illustrated on laser angioplasty

Cavitation effects in pulsed laser ablation can cause severe deformation of tissue near the ablation site. In angioplasty, they result in a harmful dilatation and invagination of the vessel walls. We suggest to reduce cavitation effects by dividing the laser pulse energy into a pre-pulse with low and an ablation pulse with high energy. The pre-pulse creates a small cavitation bubble which can be filled by the ablation products of the main pulse. For suitable energy ratios between the pulses, this bubble will not be enlarged by the ablation products, and the maximal bubble size remains much smaller than after a single ablation pulse. The concept was analyzed by numerical calculations based on the Gilmore model of cavitation dynamics and by high-speed photography of the effects of single and double pulses performed with a silicone tube as vessel model. The use of double pulses prevents the deformation of the vessel walls. The concept works with an energy ratio of up to about 1:30 between the pulses. For the calculated optimal ratio of 1:14.6, the bubble volume is reduced by a factor of 17.7. The ablation pulse is best applied when the pre-pulse bubble is maximally expanded, but the timing is not very critical.     

Direct observation of the temperature field during ablation of materials by multiple femtosecond laser pulses

We report a direct observation of the temperature field on a steel specimen during ablation by multiple femtosecond laser pulses using an infrared thermography technique. From the experimental results and simulation study of the temperature field, we quantified the deposited thermal power into the specimen during the ablation process. We found that more than two thirds of the incident laser power was deposited in the steel specimen when ablated by multiple femtosecond laser pulses. This result provides further understanding of the heating effect in materials processing by ultrashort laser pulses.     

Picosecond laser ablation of thin copper films

The ablation process of thin copper films on fused silica by picosecond laser pulses is investigated. The ablation area is characterized using optical and scanning electron microscopy. The single-shot ablation threshold fluence for 40 ps laser pulses at 1053 nm has been determinated toF _thres = 172 mJ/cm². The ablation rate per pulse is measured as a function of intensity in the range of 5 × 10⁹ to 2 × 10¹¹ W/cm² and changes from 80 to 250 nm with increasing intensity. The experimental ablation rate per pulse is compared to heat-flow calculations based on the two-temperature model for ultrafast laser heating. Possible applications of picosecond laser radiation for microstructuring of different materials are discussed.     

Selective ablation of thin films with short and ultrashort laser pulses

Micromachining of CuInSe₂ (CIS)-based photovoltaic devices with short and ultrashort laser pulses has been investigated. Therefore, ablation thresholds and ablation rates of ZnO, Mo and CuInSe₂ thin films have been measured for irradiation with nanosecond laser pulses of ultraviolet and visible light and subpicosecond laser pulses of a Ti:sapphire laser. The experimental results were compared to the theoretical evaluation of the samples heat regime. In addition, the cells photo-electrical properties were measured before and after laser machining. Scanning electron microscopy (SEM) and energy dispersive X-ray (EDX) analyses were employed to characterise the laser-induced ablation channels. Using nanosecond laser pulses, two phenomena were found to limit the laser-machining process. Residues of Mo that were projected onto the walls of the ablation channel and the metallization of the CuInSe₂ semiconductor close to the channel lead to a shunt. The latter causes the decrease of the photovoltaic efficiency. As a consequence of these limiting effects, only subpicosecond laser pulses allowed the selective or complete ablation of the thin layers without a relevant change of the photo-electrical properties.     

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     

A study of blast waveforms detected simultaneously by a microphone and a laser probe during laser ablation

We examine blast waves generated in air during irradiation of absorbing samples with Nd: YAG laser pulses of fluences exceeding the ablation threshold. Blast waves were detected simultaneously by a wideband microphone and a laser beam deflection probe. By a comparative analysis of both signals in the time and frequency domain we investigate characteristic features of their nonlinear waveform evolution. To explain the observed phenomena we employ the weak shock solution of the point explosion model.     

Femtosecond laser ablation of aluminium

We investigate femtosecond laser ablation of aluminium using a hybrid simulation scheme. Two equations are solved simultaneously: one for the electronic system, which accounts for laser energy absorption and heat conduction, the other for the dynamics of the lattice where the ablation process takes place. For the electron-temperature a generalized heat-conduction equation is solved by applying a finite difference scheme. For the lattice properties, e.g. pressure, density or temperature, we use common molecular dynamics. Energy transfer between the subsystems is allowed by introducing an electron-phonon coupling term. This combined treatment of the electronic and atomic systems is an extension of the well known two-temperature model [Anisimov, Kapeliovich, Perel’man, Electron emission from metal surfaces exposed to ultra short laser pulses, JETP Lett. 39 (2)].     

The influence of thermal diffusion on laser ablation of metal films

Single-shot ablation thresholds of nickel and gold films in the thickness range from 50 nm to 7 m have been measured for 14 ns laser pulses at 248 nm, using photoacoustic shock wave detection in air. The metal films were deposited on fused silica substrates. The ablation threshold was found to increase linearly with film thickness up to the thermal diffusion length of the film. Beyond this point it remains independent of film thickness. The proportionality between threshold fluence and thickness allows the prediction of ablation thresholds of metal films from the knowledge of their optical properties, evaporation enthalpies and thermal diffusivities. Physically it proves that ablation is driven by the energy density determined by the thermal diffusion length. A simple thermodynamic model describes the data well. Thermal diffusivities, an essential input for this model, were measured using the technique of transient thermal gratings. In addition, the substrate dependence of the ablation threshold was investigated for 150 nm Ni films.     

Effects of laser operating parameters on metals micromachining with ultrafast lasers

180 femtoseconds (1 kHz) and 10 picoseconds (1-50 kHz) ultrafast laser micro-structuring of the metals Ti alloy, Al and Cu have been studied for the purpose of industrial application. The effects of some key laser operating parameters were investigated. The evolution of surface morphology revealed that laser pulses overlap in a range around the spatial FWHM can help to achieve optimal residual surface roughness. While observed ablation rate (unit: μm³ per pulse) changed dramatically with repetition rate due to the combined effects of plasma absorption, residual thermal energy and phase transition, higher throughput can be achieved with higher repetition rate. This study also indicated that residual surface roughness is almost independent of repetition rate at 10 ps temporal pulse length. The ablation depth is approximately proportional to the number of overscan; however, machining accuracy deteriorates, especially for femtosecond laser processing and metals with low thermal conductivity and short electron-phonon coupling time.     

Silicon surface morphology study after exposure to tailored femtosecond pulses

Temporal pulse shaping of ultrashort laser pulses has been used for laser ablation of semiconductors. Even the simplest double pulse sequence with a delay of several picoseconds shows remarkable differences in the interaction process, compared to a single pulse of the same total energy. We discuss the interaction of double pulses with single crystal silicon sample in the context of crater morphology for multiple pulses on the same spot. The growth of the typical columnar structures in helium at atmospheric pressure is suppressed and the crater bottom is flat despite the Gaussian beam profile. The influence of the temporal pulse shape has to be treated in conjunction with the influence of the other ablation parameters.     

Exploration of pulse timing for multiple laser hits within a combined heat transfer, phase change, and gas dynamics model for laser ablation

Laser ablation involves heat transfer, phase changes and/or chemical reactions, and gas dynamics. All three of these processes are tightly coupled with each other. A model has previously been developed to simulate the nanosecond scale laser ablation of carbon. This model has been extended to accommodate longer term simulations and multiple laser pulses. The effects of varying the timing of a second laser pulse by tens of nanoseconds are explored. It is shown that by changing this interval one can control the total mass ablated and the mass transfer rate.     

Thermal model for nanosecond laser sputtering at high fluences

The vaporization effect and the following plasma shielding generated by high-power nanosecond pulsed laser ablation are studied in detail based on the heat flux equation. As an example of Si target, we obtain the time evolution of the calculated surface temperature, ablation rate and ablation depth by solving the heat flow equations using a finite difference method. It can be seen that plasma shielding plays a more important role in the ablation process with time. At the same time, the variation of ablation depth per pulse with laser fluence is performed. Our numerical results are more agreed with the experiment datum than other simulated results. The result shows that the plasma shielding is very important.     

Femtosecond laser-induced formation of spikes on silicon

We find that silicon surfaces develop arrays of sharp conical spikes when irradiated with 500-fs laser pulses in SF₆. The height of the spikes decreases with increasing pulse duration or decreasing laser fluence, and scales nonlinearly with the average separation between spikes. The spikes have the same crystallographic orientation as bulk silicon and always point along the incident direction of laser pulses. The base of the spikes has an asymmetric shape and its orientation is determined by the laser polarization. Our data suggest that both laser ablation and laser-induced chemical etching of silicon are involved in the formation of the spikes. Received: 10 September 1999 / Accepted: 7 January 2000 / Published online: 8 March 2000