Cent. Eur. J. Phys. • 6(2) • 2008 • 327-331 DOI: 10.2478/s11534-008-0026-0 Central European Journal of Physics Impact of the laser wavelength and fluence on the ablation rate of aluminium Research Article Mihai Stafe12∗ , Ionut Vladoiu1 , Ion M. Popescu1 1 Department of Physics, University “Politehnica” of Bucharest, Spl. Independendei 313, 060042 Bucharest, Romania 2 Present address: Department of Experimental Physics, University of Szeged, Dom ter 9, H-6720 Szeged, Hungary Received 29 Jun 2007; accepted 3 December 2007 Abstract: 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. PACS (2008): 52.38.Mf, 42.62.-b, 81.05.Bx, 79.20.Ds Keywords: ablation rate • nanosecond laser pulses • metal © Versita Warsaw and Springer-Verlag Berlin Heidelberg. 1. Introduction The efficiency of material removal under the action of short, intense laser pulses is described by the ablation rate, which gives the maximum thickness of the layer ablated during irradiation with a laser pulse. Understanding and controlling the ablation rate is essential for micro∗ E-mail: [email protected] patterning and pulsed laser-deposition in electronics, optoelectronics, and micromechanics, where the ablation rate is a key parameter [1–7]. The ablation rate is strongly influenced by the thermal and optical properties of the processed material (e.g., mass density, surface reflectivity, optical absorptivity, thermal conductance) [1–6, 8, 9], ambient conditions [2, 9, 10], and by the characteristics of the processing laser beam (e.g., pulse duration, number of pulses, energy, fluence, wavelength) [1, 2, 5, 6, 11–18]. Due to their being cost effective, there is an ongoing effort to develop new techniques 327 Unauthenticated Download Date | 6/18/17 8:48 PM Impact of the laser wavelength and fluence on the ablation rate of aluminium based on nanosecond laser ablation, and to determine the optimum parameters of the nanosecond laser-pulses that allow one to obtain high quality micropatterns on different metallic or non-metallic materials [8–10, 19–22]. The experiments indicate that the ablation rate increases logarithmically with the fluence of the nanosecond pulses in the case of semiconductors and dielectrics [2, 5, 16], while for values of the fluence higher than a threshold there is a steep increase of the ablation rate [16, 19–21]. The wavelength of the laser has a significant influence on the ablation rate: the shorter the wavelength, the higher the ablation rate. The dependence of the ablation rate on the laser wavelength is mainly due to the superposition of three inter-related phenomena: the decrease of the intrinsic absorptivity of dielectrics and semiconductors, the increase of the surface reflectivity, and the enhancement of the absorptivity of the laser-produced plasma with increasing the laser wavelength. Here, we investigate the dependence of the ablation rate of aluminium on the fluence of nanosecond laser pulses in ambient atmosphere conditions, using nanosecond pulses at 1064 nm and 532 nm wavelengths. The fluence at the surface of the metallic target surface is varied by changing the diameter of the laser beam in the focal plane of a lens. We demonstrate that the ablation rate is approximately one order of magnitude higher for the visible pulses, and the threshold fluence that marks a jump of the ablation rate is three-fold higher in the case of pulses at 532 nm as compared to the 1064-nm wavelength pulses. 2. Experiments The experimental setup consists of a Q-switched Nd-YAG laser system, a focusing lens and an aluminium target placed perpendicular to the laser beam. The experiments were carried out in ambient atmosphere conditions. The laser system works in the TEM00 mode and generates fundamental pulses at 1064 nm wavelength which can be frequency doubled (532 nm wavelength) by sending them through a second harmonic generator module. The laser pulses are characterized by a duration of 4.5 ns, repetition rate of 10 Hz, and energies of 360 mJ/pulse and 180mJ/pulse for the fundamental and second harmonic pulses, respectively. The laser pulses are focused at normal incidence on a 1 mm-thick aluminium plate by a focusing lens system. The target is first placed in the focal plane of the convergent lens (f/10, f=10 cm) giving a diameter of the irradiated area of 1 mm and 0.4 mm for the fundamental and second harmonic pulses, respectively. Consequently, the fluence at the target surface was approximately 20 J/cm2 and 100 J/cm2 for the two wavelengths. To vary the fluence of the laser beam we varied the diameter of the irradiated area by moving the target away from the focal plane. To avoid the effect of air breakdown that would lead to the waste of laser energy in heating the plasma plume ignited in front of the sample, the aluminium target is translated axially toward the incoming laser beam. The translation of the target is done with micrometric resolution by using a mechanical stage on which the sample is fixed. The sample is translated with increments (along the axial direction) of 5 mm and 2 mm for pulses at 1064 nm and 532 nm wavelengths, respectively. The increment steps for translating the sample were chosen such that the relative variation of the diameter of the irradiated area from one position to the other is approximately the same at the two wavelengths. Thus, the diameter of the irradiated area increases from its minimum value in the focal plane up to 2.5 mm and 1.6 mm for the two wavelengths, while the corresponding fluence decays from its maximum value in the focal plane down to 6 J/cm2 in both cases. Because the diameter of the crater is higher than its depth (the aspect ratio is < 1), the ablation can be considered as one-dimensional and, consequently, the diameter of the irradiated area could be approximated by the diameter of the crater that is drilled into the aluminium target [9, 22]. The fluence was then determined by dividing the energy of the pulse by the irradiated area [9]. The dependence of the ablation rate on the laser fluence was derived from the depth of the craters that are drilled in multiple-pulse regime into the aluminium target at each particular position along its axial path. Because the ablation rate usually depends on the number of consecutive laser pulses [2, 14], we determined the number of laser pulses for drilling a crater such that the ablation rate is approximately constant for each successive laser pulse. Our measurements indicate that 200 fundamental pulses and 10 second harmonic pulses ensure an approximately constant ablation rate and, moreover, enable us to obtain a crater sufficiently deep to allow measurement of the ablation rate with a relative error of maximum 5%. The ablation rate was then calculated by dividing the depth of the crater depth by the number of laser pulses that irradiated the target for drilling the crater. The depths and the diameters of the craters were measured using a metallographic microscope with micrometric resolution. 3. Results and discussion The dependence of the ablation rate (∆h) of aluminium on the fluence (F ) of the fundamental and second harmonic pulses is depicted in Figs. 1, 2, 3, 4. 328 Unauthenticated Download Date | 6/18/17 8:48 PM Mihai Stafe, Ionut Vladoiu, Ion M. Popescu whereas for the for the pulses at 1064 nm wavelength, the fitting curve is ∆h = 0.1 ln[1.05 F (J/cm2 )] (µm). Figure 1. Ablation rate of aluminium in open air as a function of laser fluence of a 4.5 ns laser pulse. The laser wavelength is 532 nm. For the case of the second harmonic pulses, the increase of the fluence to a value of ∼50 J/cm2 leads to an approximately logarithmic increase of the ablation rate to a maximum of ∼6 µm/pulse (Fig. 1). In a similar manner, for the fundamental laser pulses, the increase of the fluence to ∼15 J/cm2 leads to an approximately logarithmic increase of the ablation rate to a maximum of ∼0.3 µm/pulse (Fig. 3). In the case of the pulses at 532 nm wavelength, the fitting curve is described by the equation The maximum ablation rate is approximately one order of magnitude higher when the target is irradiated with second harmonic pulses instead of fundamental pulses. The much higher efficiency of the ablation in the case of second harmonic pulses is likely due to the superposition of three phenomena. First, the increase of the optical absorptivity of aluminium upon decreasing the wavelength [2, 5] leads to strong localized heating and, consequently, to a high ablation rate. Second, since the surface of the target surface appears to be covered with a very compact slag-layer after irradiation with infrared pulses, the oxidation of the surface during the interval between the laser pulses could lead to a further decay of the intrinsic absorptivity of the target for laser pulses at 1064 nm wavelength as compared to those at 532 nm [2, 9]. Third, the dependence of the absorption coefficient of plasma (αIB ) on the wavelength (λ) αIB ≈ λ3 Ablation rate of aluminium in open air as a function of laser fluence of a 4.5 ns laser pulse. The laser wavelength is 532 nm. The dashed lines indicate the fitting curves for the ablation rate vs fluence for values of the fluence smaller than the threshold. ∆h = 1.1 ln[5.85 F (J/cm2 )] (µm) (1) (3) implies that the absorption of the laser beam into the ignited plasma plume via the inverse-Bremstrahlung effect is significantly stronger in the case of longer wavelengths [2, 5, 11, 23]. As a consequence, the plasma produced by the leading edge of an infrared pulse becomes much more absorbing and efficiently reflective for the remaining pulse as compared to a visible pulse. This prevents the infrared pulse from reaching the target surface and producing further ablation shortly after the onset of the pulse. A jump of the ablation rate is observed for a threshold value of the fluence Fth , which is ∼50 J/cm2 for the second harmonic, and ∼15 J/cm2 for the fundamental pulses. Further increase of the fluence above the threshold value leads to a steep increase of the ablation rate at both wavelengths (Figs. 2, 4). In the case of visible pulses, the steep increase can be approximated by an exponential function (Fig. 2): ∆h = 4.1 exp[0.007 F (J/cm2 )] (µm). Figure 2. (2) (4) The results above on the existence of a threshold fluence and the steep increase of the ablation rate upon increasing the fluence above the threshold value are consistent with previous work on metallic and non-metallic materials in different irradiation conditions [16, 19–21]. There, ablation was performed in vacuum conditions, and the fluence was varied via the pulse energy. Values of the threshold 329 Unauthenticated Download Date | 6/18/17 8:48 PM Impact of the laser wavelength and fluence on the ablation rate of aluminium Figure 3. Ablation rate of aluminium in open air as a function of laser fluence of a 4.5 ns laser pulse. The laser wavelength is 1064 nm. fluence were reported in the range of 5 − 25 J/cm2 , and it was suggested that the existence of a threshold fluence is mainly due to phase explosion [16, 19–21]. For the particular case assessed here, the jump of the ablation rate is likely due to the following two causes. First, because the increase of the ablation rate is accompanied by a significant amount of bright sparks that emerge into the plume, the jump of the ablation rate is likely related to the transition from a normal vaporization regime of the irradiated sample (which is characterized by a small mass-removal rate) to a phase-explosion regime (which is characterized by ejection of small particulates and melt droplets and an enhanced mass-removal rate). The ejection of droplets is enhanced by the recoil pressure exerted by the plasma plume onto the melted surface [24], such that the infrared pulses (which heat the plasma stronger) could start the ejection process at a lower threshold fluence (∼15 J/cm2 ) as compared to the visible pulses (∼50 J/cm2 ). The second cause contributing to the jump in the ablation rate consists in the change of the dimensionality of the hydrodynamics of the plasma plume from one-dimensional to three-dimensional. In the one-dimensional regime the expansion of the plasma-plume is mainly axial, being characterized by high density and strong absorptivity. In constrast, in the three-dimensional regime the plasma plume expands in both axial and radial directions, and is characterized by low density and weak absorptivity [5]. The jump appears when the diameter of the laser beam (central Airy disk) becomes the same order of magnitude with the hydrodynamic length of the laser-produced plasma. This relationship between the beam diameter and the hydrodynamic length of the plasma at threshold is demonstrated as follows. For an usual plasma temperature of 105 K [11], Figure 4. Ablation rate of aluminium in open air as a function of laser fluence of a 4.5 ns laser pulse. The laser wavelength is 1064 nm. The dashed lines indicate the fitting curves for the ablation rate vs fluence for values of the fluence smaller than the threshold. The dotted line indicates the steep increase of the ablation rate with fluence for values of the fluence above the threshold. the plasma hydrodynamic length [2, 11], lh = vp τ (5) is ∼50 µm, which is similar to the diameter of the laser beam corresponding to the threshold fluences Fth of either visible or infrared pulses. In equation (5), vp = p γ kB Tp /M is the expansion velocity of the plasma plume considered as an ideal gas with adiabatic coefficient γ = 5/3, temperature Tp and the atomic mass M, τ is the pulse duration, and kB is the Boltzmann constant. 4. Conclusion The impact of the fluence and wavelength of the nanosecond laser pulses on the ablation rate of aluminium was investigated in ambient atmosphere conditions. We varied the fluence of the laser pulses by changing the diameter of the irradiated area at the target surface, and the wavelength by using the fundamental and the second harmonic beams of a Q-switched Nd-YAG laser system. The results indicate that the ablation rate has an approximately logarithmic increase with the fluence for ablation rates smaller than ∼6 µm/pulse and ∼0.3 µm/pulse when using pulses at 532 nm and 1064 nm wavelengths, respectively. The much higher efficiency of the ablation in the case of second harmonic pulses as compared to the fundamental pulses is due to the superposition of the following three effects: the increase of the optical absorptivity of 330 Unauthenticated Download Date | 6/18/17 8:48 PM Mihai Stafe, Ionut Vladoiu, Ion M. Popescu aluminium with decreasing wavelength, the weaker oxidation of the surface of the target when irradiated at short wavelengths, and the decay of the plasma absorption via the inverse-Bremstrahlung effect at short wavelengths. The increase of the fluence to a threshold value of ∼50 J/cm2 for the second harmonic pulses, and ∼15 J/cm2 for the fundamental pulses, leads to a jump of the ablation rate. Further increase of the fluence above the threshold value leads to a steep increase of the ablation rate at both wavelengths. In the case of visible pulses, the steep increase of the ablation rate with the fluence above the threshold fluence can be described by an exponential function. The jump of the ablation rate at the threshold fluence is likely due to the superposition of two effects. First, the appearance of a significant number of bright sparks (particulates and melted material) within the plasma plume indicates a transition from the normal vaporization to phase explosion with increasing the fluence of the pulses above the threshold value. 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