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     

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.     

Influence of consecutive picosecond pulses at 532 nm wavelength on laser ablation of human teeth

The interaction of 40 ps pulse duration laser emitting at 532 nm wavelength with human dental tissue (enamel, dentin, and dentin–enamel junction) has been investigated. The crater profile and the surface morphology have been studied by using a confocal auto-fluorescence microscope (working in reflection mode) and a scanning electron microscope. Crater profile and crater morphology were studied after applying consecutive laser pulses and it was found that the ablation depth increases with the number of consecutive pulses, leaving the crater diameter unchanged. We found that the thermal damage is reduced by using short duration laser pulses, which implies an increased retention of restorative material. We observe carbonization of the irradiated samples, which does not imply changes in the chemical composition. Finally, the use of 40 ps pulse duration laser may become a state of art in conservative dentistry.     

Material ablation and plasma state for single and collinear double pulses interacting with iron samples at ambient gas pressures below 1 bar

The influence of the ambient gas pressure on ablated material and the plasma state of laser-inducedplasmas using single and collinear double pulses is studied. A Q-switchedNd:YAG laser pulse is focused on iron samples in air at pressures ranging from 0.1 to 1013 mbar. At 1013 mbar double pulses ablate up to a factor of 4.6 more material than single pulses of the same energy. Whereas between 1013 mbar and 100 mbar a strong variation of the ablation ratio is found, the pressure dependence vanishes below 100 mbar. Electron densities in the plasma are always higher for single pulses and increase monotonously with higher ambient pressures. While the electron density for single and double pulses at 1013 mbar is close to the same value of about 10¹⁷ cm^-3, the electron temperature is more than 1500 K higher for double pulses. The plasma state achieved with double pulses at atmospheric pressure is similar to that obtained with single pulses of the same energy at a pressure of 100 mbar. Thus the effect of double pulses can be interpreted as a “laser-generated vacuum” in terms of the formation of a transient localized low particle density region in the interaction region. PACS 52.38.Mf; 78.47.+p; 42.62.Fi     

Femtosecond laser ablation characteristics of nickel-based superalloy C263

Femtosecond laser (180 fs, 775 nm, 1 kHz) ablation characteristics of the nickel-based superalloy C263 are investigated. The single pulse ablation threshold is measured to be 0.26±0.03 J/cm² and the incubation parameter ξ=0.72±0.03 by also measuring the dependence of ablation threshold on the number of laser pulses. The ablation rate exhibits two logarithmic dependencies on fluence corresponding to ablation determined by the optical penetration depth at fluences below ∼5 J/cm² (for single pulse) and by the electron thermal diffusion length above that fluence. The central surface morphology of ablated craters (dimples) with laser fluence and number of laser pulses shows the development of several kinds of periodic structures (ripples) with different periodicities as well as the formation of resolidified material and holes at the centre of the ablated crater at high fluences. The debris produced during ablation consists of crystalline C263 oxidized nanoparticles with diameters of ∼2–20 nm (for F=9.6 J/cm²). The mechanisms involved in femtosecond laser microprocessing of the superalloy C263 as well as in the synthesis of C263 nanoparticles are elucidated and discussed in terms of the properties of the material.     

Crater geometry characterization of Al targets irradiated by single pulse and pulse trains of Nd:YAG laser in ambient air and water

High intensities laser pulses are capable to generate a crater when irradiating metal targets. In such condition, after each irradiation significant ablation occurs on the target surface and as a result a crater is formed. The crater characterization is very important specifically for some applications such as micromachining. In this paper, the crater formation in metal targets was studied experimentally. The planar aluminum 5052 targets were irradiated by frequency doubled (532 nm), Q-switched Nd:YAG (∼6 ns) laser beam in ambient air and distilled water. A crater was produced after each irradiation and it was characterized by an optical microscope. Different laser intensities as well as pulse trains were applied for crater formation. The effects of laser characteristics in crater geometry were examined. The depth of the craters was measured by optical microscope and the diameter (width) was characterized by processing of the crater image. The results were explained in terms of ablation threshold and plasma shielding. The results show that the crater geometry extremely depends on the laser pulse intensity, the number of laser pulses, and ambient.     

Experimental investigation of ablation efficiency and plasma expansion during femtosecond and nanosecond laser ablation of silicon

Femtosecond laser (Ti:sapphire, 100 fs pulse duration) ablation of silicon in air was compared with nanosecond laser (Nd:YAG, 3 ns pulse duration) ablation at ultraviolet wavelength (266 nm). Laser ablation efficiency was studied by measuring crater depth as a function of pulse number. For the same number of laser pulses, the fs-ablated crater was about two times deeper than the ns-crater. The temperature and electron number density of the laser-induced plasma were determined from spectroscopic measurements. The electron number density and temperature of fs-induced plasmas decreased faster than ns-induced plasmas due to different energy deposition mechanisms. Images of the laser-induced plasma were obtained with femtosecond time-resolved laser shadowgraph imaging. Plasma expansion in both the perpendicular and the lateral directions were compared. PACS 52.38.Mf; 52.30.-q     

High rate deep channel ablative formation by picosecond-nanosecond combined laser pulses

Temporally profiled pulsed radiation of the Nd:YAG laser was applied to drilling and micromachining of ceramics, steel, and CVD diamond, demonstrating one or two orders of magnitude enhancement of ablation rates compared to conventional pico- and nanosecond-pulsed ablation at the same energy density. The developed laser system delivered combined pulses consisting of a picosecond pulse train followed by a nanosecond pulse train. The combination of picosecond and nanosecond components within one laser shot turned out to be especially beneficial for high-aspect-ratio channel formation. Polarization dependence of the ablated deep crater morphology was observed in AlN samples. Waveguide radiation propagation in self-made deep channels as well as the influence of high-temperature laser-produced plasma on this phenomena are discussed.     

Formation of cavitation-induced pits on target surface in liquid-phase laser ablation

It is well known that a crater is formed on the target surface by the irradiation of intense laser pulses in laser ablation. In this work, we report that additional pits are formed on the bottom surface of the ablation crater due to the collapse of a cavitation bubble in liquid-phase laser ablation. We observed the formation of several cavitation-induced pits when the fluence of the laser pulse used for ablation was approximately 5 J/cm². The number of cavitation-induced pits decreased with the laser fluence, and we observed one or two cavitation-induced pits when the laser fluence was higher than 10 J/cm². In addition, we examined the influence of the liquid temperature on the formation of cavitation-induced pits. The collapse of the cavitation bubble was not observed when the liquid temperature was close to the boiling temperature, and in this case, we found no cavitation-induced pits on the bottom surface of the ablation crater. This experimental result was discussed by considering the cavitation parameter.     

Simulation of ultrashort double-pulse laser ablation

In this paper, we study the mechanisms of femtosecond double-pulse laser ablation of metals. It was previously shown experimentally that the crater depth monotonically drops when the delay between two successive pulses increases. For delays longer than the time of electron-ion relaxation the crater depth can be even smaller than that produced by a single pulse. The results of the performed hydrodynamic simulation show that the ablation can be suppressed due to the formation of the second shock wave. The modeling results of the double-pulse ablation obtained for different delays correlate with the experimental findings.     

Thermal characteristics of double-layer thin film target ablated by femtosecond laser pulses

Thermal characteristics of tightly-contacted copper--gold double-layer thin film target under ablation of femtosecond laser pulses are investigated by using a two-temperature theoretical model. Numerical simulation shows that electron heat flux varies significantly on the boundary of copper--gold film with different maximal electron temperature of 1.15×10³ K at 5 ps after ablating laser pulse in gold and copper films, which can reach a balance around 12.6 ps and 8.2 ps for a single and double pulse ablation, respectively, and in the meantime, the lattice temperature difference crossing the gold--copper interface is only about 0.04×10³ K at the same time scale. It is also found that electron--lattice heat relaxation time increases linearly with laser fluence in both single and double pulse ablation, and a sudden change of the relaxation time appears after the laser energy density exceeds the ablation threshold.     

Simulation of laser ablation in aluminum: the effectivity of double pulses

Lasers are becoming a more and more important tool in cutting and shaping materials. Improving precision and effectivity is an ongoing demand in science and industry. One possibility is double pulses. Here, we study laser ablation of aluminum by the two-temperature model. There the laser is modeled as a source in a continuum heat conduction equation for the electrons, whose temperature then is transferred to a molecular dynamics particle model by an electron–phonon coupling term. The melting and ablation effectivity is investigated depending on the relative intensity and the time delay between two Gaussian shaped laser pulses. It turns out that at least for aluminum the optimal pulse shapes are standard Gaussian pulses. For double pulses with delay times up to 200 ps, we find a behavior as observed in experiment: The ablation depth decreases beyond a delay of 10 ps even if one does not account for the weakening at the second pulse due to laser–plasma interaction.     

Diffuse X-ray scattering near a two-dimensional solid–liquid phase transition at the <Emphasis Type="Italic">n</Emphasis>-hexane–water interface

Spatial profiles of single-shot microcraters produced by tightly focused femtosecond laser pulses with variable pulse energies are measured by means of a laser confocal microscope. Dependences of crater depth on laser intensity at different pulse energies appear as overlapping saturating curves with the same threshold, indicating the presence of nonlinear absorption and absence of nonlocal ablation effects. A monotonic twofold increase in absorption nonlinearity is related to the transition from minor defect-band absorption to fundamental band-to-band absorption.     

Microdrilling of metals with an inexpensive and compact ultra-short-pulse fiber amplified microchip laser

We have investigated the ultra-fast microdrilling of metals using a compact and cheap fiber amplified passively Q-switched microchip laser. This laser system delivers 100-ps pulses with repetition rates higher than 100 kHz and pulse energies up to 80 μJ. The ablation process has been studied on metals with quite different thermal properties (copper, carbon steel and stainless steel). The dependence of the ablation depth per pulse on the pulse energy follows the same logarithmic scaling laws governing laser ablation with sub-picosecond pulses. Structures ablated with 100-ps laser pulses are accompanied only by a thin layer of melted material. Despite this, results with a high level of precision are obtained when using the laser trepanning technique. This simple and affordable laser system could be a valid alternative to nanosecond laser sources for micromachining applications.     

飞秒双脉冲激光照射金属薄膜的热行为

通过双温方程对飞秒单脉冲与双脉冲照射金薄膜进行了计算模拟分析,得到了金靶的电子温度和晶格温度随着时间空间的变化。在同样激光能量密度下,单脉冲与双脉冲使得金膜温度的变化表明双脉冲使得更多的激光能量渗透到靶材内部,这些能量可以使得烧蚀深度更深,有利于提高激光烧蚀靶材的效率。计算结果显示随着激光能量密度的增加熔化面深度逐渐增加,单脉冲与双脉冲熔化面深度的变化明显不同。在激光能量密度高于损伤阈值附近,单脉冲的烧蚀深度大于双脉冲的烧蚀深度,随着激光能量密度增加,双脉冲的烧蚀深度将大于单脉冲的烧蚀深度。     

Electron dynamics triggered by double attosecond pulses: Simulations based on time-dependent density functional theory

In order to observe the high-field effect, the external laser field must reach its peak intensity before the electron ionization. To this end, it is important to reduce pulse duration to typical attosecond timescale. In this paper, the interaction electron dynamics between attosecond pulses and dielectric is investigated within the time-dependent density functional theory. Taking the CaF₂ crystal as an example, we give a comparison of electron dynamics response between single and double pulses. Moreover, the nonlinear energy absorption and electron excitation processes are simulated by adjusting the polarization direction of the sub-pulse. Present results demonstrate that the double pulses show lower electron excitation and energy absorption than the single pulse, which is in accordance with experimental higher ablation threshold and smaller heat-affected zones of the double pulses. In addition, the curves of final excited electron number and energy absorption exhibit the quasi-symmetry about the axis of 180°, which has not been reported yet.     

Drilling enhancement by nanosecond-nanosecond collinear dual-pulse laser ablation of titanium in vacuum

Laser ablation of titanium in vacuum was performed using single- and dual-pulse regime in order to study crater formation. Crater profiles were analyzed by optical microscopy. It was found that the repetition-rate plays an important role in a process of laser ablation. The drilling is most effective for the highest repetition-rate. For the same total number of laser pulses clear drilling enhancement was achieved by dual-pulse regime of ablation in comparison to single-pulse regime. The strongest ablation rate in dual-pulse regime was achieved for the delay time between the pulses τ = 370 ns. Results are discussed in terms of decreased ablation threshold due to continuous heating of the target during the experiment.     

Robust plasmonic substrates

We report on resonant infrared laser ablation of polystyrene using single 8 ps pulses at a wavelength of 3.31 μm generated by a MgO:PPLN optical parametric amplifier pumped by a Nd:YLF laser. We determined the single-pulse ablation threshold to be 0.46 J/cm², about a factor of five smaller than in previous free-electron-laser studies. Time-resolved imaging of the laser–target interaction reveals that the detailed dynamics of the ablation process begin with thermal expansion of a large volume of hot material from which a less dense plume of polymeric material evaporates. This plume disappears on a time scale of 0.75 μs and the hot polymer material recedes back into the crater from which it was expelled. Subsequently, and on a much longer time scale, structural alterations in the ablation crater continue to evolve for at least another millisecond. Our results suggest that single picosecond pulses are effective for the ablation of polymers and exhibit dynamics similar to those observed in studies using a free-electron laser.     

Morphology of ablation craters generated by fs laser pulses in LiNbO3

The surface morphology of the ablation craters generated in LiNbO₃ by 130 fs laser pulses at 800 nm has been investigated by AFM/SNOM microscopy. The single pulse fluence corresponding to the ablation threshold has been estimated to be ≈1.8 J/cm².A complex structure including random cone-shaped protrusions is observed inside the ablated crater. The scale of the protrusion spacing is in the submicron range and the heights are typically of a few tens of nanometers. At and outside the crater rim a novel quasi-periodic wave-like topography pattern is observed in both types of microscopy techniques. The average wavelength, that is slightly dependent on pulse fluence, is (500-800 nm) comparable to the light wavelength. This novel topography feature keeps a close similarity with a Fresnel diffraction pattern by an absorbing circular obstacle or impact wave pattern produced by a combination of heat and shock wave (resemble that of impact crater). It is proposed that the obstacle is associated to the strongly nonlinear multiphoton absorption at the peak of the pulse profile. The energy deposited by nonlinear absorption of such profile causes ablation of both the crater and the rippled structure.     

Raman study of phase transformation of TiO2 rutile single crystal irradiated by infrared femtosecond laser

Titanium dioxide (TiO₂) rutile single crystal was irradiated by infrared femtosecond (fs) laser pulses with repetition rate of 250 kHz and phase transformation of rutile TiO₂ was observed. Micro-Raman spectra show that the intensity of E_g Raman vibrating mode of rutile phase increases and that of A_1g Raman vibrating mode decreases apparently within the ablation crater after fs laser irradiation. With increasing of irradiation time, the Raman vibrating modes of anatase phase emerged. Rutile phase of TiO₂ single crystal is partly transformed into anatase phase. The anatase phase content transformed from rutile phase increased to a constant with increasing of fs pulse laser irradiation time. The study indicates the more stable rutile phase is transformed into anatase phase by the high pressure produced by fs pulse laser irradiation.