Ultrashort-pulse laser ablation of indium phosphide in air

Ablation of indium phosphide wafers in air was performed with low repetition rate ultrashort laser pulses (130 fs, 10 Hz) of 800 nm wavelength. The relationships between the dimensions of the craters and the ablation parameters were analyzed. The ablation threshold fluence depends on the number of pulses applied to the same spot. The single-pulse ablation threshold value was estimated to be φ_th(1)=0.16 J/cm². The dependence of the threshold fluence on the number of laser pulses indicates an incubation effect. Morphological and chemical changes of the ablated regions were characterized by means of scanning electron microscopy and Auger electron spectroscopy. Received: 30 May 2000 / Accepted: 31 May 2000 / Published online: 23 August 2000     

Control of material removal of fused silica with single pulses of few optical cycles to sub-picosecond duration

Surface ablation of a dielectric material (fused silica) by single femtosecond pulses is studied as a function of pulse duration (7–450 fs) and applied fluence (F _th<F<10F _th). We show that varying the pulse duration gives access to high selectivity (with resolution ∼10 nm) for axial removal of matter but does not influence the transverse ablation selectivity, which only depends on the normalized applied fluence F/F _th. The ablation efficiency is shown to be inversely dependent on the pulse duration and saturates with respect to the applied fluence earlier at ultra-short pulse durations (≤30 fs). The deduced optimal fluence F _opt corresponding to the highest ablation efficiency for each pulse width defines two regimes of laser application. Below F _opt, the removed material depth can be accurately adjusted in a large range (∼40–200 nm) as a function of the applied fluence and the morphology of the ablated pattern almost reproduces the Gaussian beam distribution. Above F _opt, the material removal depth tends to saturate and the morphology of the ablated pattern evolves to a top-hat distribution. The coupled evolution of depth and morphology is related to the dynamics of formation of dense plasma at the surface of the material, acting as an ultra-fast optical shutter.     

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.     

The growth of Y2SiO5:Ce thin films with pulsed laser deposition

Y₂SiO₅:Ce phosphor thin films were grown onto Si(100) substrates with pulsed laser deposition (PLD) using a 248-nm KrF excimer laser. Process parameters were varied during the growth process and the effect on the surface morphology and cathodoluminescence (CL) was analysed. The process parameters that were changed included the following: gas pressure (vacuum (5×10⁻⁶ Torr), 1×1⁻² Torr and 1 Torr O₂), different gas species (O₂, Ar and N₂ at a pressure of 455 mTorr), laser fluence (1.6±0.1 J cm⁻² and 3.0±0.3 J cm⁻²) and substrate temperature (400 and 600°C). The surface morphology was investigated with atomic force microscopy (AFM). The morphology of the thin films ablated in vacuum and 10 mTorr ambient O₂ showed more or less the same trend. An increase in the pressure to 1 Torr O₂, however, showed a definite increase in deposited particle sizes. Ablation in N₂ gas resulted in small particles of 20 nm in diameter and ablation in O₂ gas produced bigger particles of 20, 30 and 40 nm as well as an agglomeration of these particles into bigger size clusters of 80 to 100 nm. Ablation in Ar gas led to particle sizes of 30 nm and the particles were much more spherically defined and evenly distributed on the surface. The higher fluence deposition led to bigger particle and grain sizes as well as thicker layers with respect to the lower fluence. The particle sizes of the higher fluence vary mainly between 130 and 140 nm and the lower fluence sizes vary between 50 and 60 nm. The higher fluence particles consist of smaller particles ranging from 5 to 30 nm as measured with AFM. The surface structure of the thin film ablated at 400°C substrate temperature is less compact (lesser agglomeration of particles than at 600°C). The increase in substrate temperature definitely resulted in a rougher surface layer. CL was measured to investigate the effect of the surface morphology on the luminescent intensities. The increased O₂ ambient (1 Torr) resulted in a higher CL intensity compared to the thin films ablated in vacuum. The thin film ablated in Ar gas showed a much higher CL intensity than the other thin films. Ablation at a high fluence resulted in a higher CL intensity. The higher substrate temperature resulted in better CL intensities. The more spherically shaped particles and rougher surface led to increase CL intensities.     

Generation of CdS clusters using laser ablation: the role of wavelength and fluence

The formation of cationic clusters in the laser ablation of CdS targets has been investigated as a function of wavelength and fluence by mass spectrometric analysis of the plume. Ablation was carried out at the laser wavelengths of 1064, 532, 355, and 266 nm in order to scan the interaction regimes below and above the energy band gap of the material. In all cases, the mass spectra showed stoichiometric Cd _n S _n ⁺ and nonstoichiometric Cd _n S _n−1⁺, Cd _n S _n+1⁺, and Cd _n S _n+2⁺ clusters up to 4900 amu. Cluster size distributions were well represented by a log-normal function, although larger relative abundance for clusters with n=13, 16, 19, 34 was observed (magic numbers). The laser threshold fluence for cluster observation was strongly dependent on wavelength, ranging from around 16 mJ/cm² at 266 nm to more than 300 mJ/cm² at 532 and 1064 nm. According to the behavior of the detected species as a function of fluence, two distinct families were identified: the “light” family containing S₂⁺ and Cd⁺ and the “heavy” clusterized family grouping Cd₂⁺ and Cd _n S _m ⁺. In terms of fluence, it has been determined that the best ratio for clusterization is achieved close to the threshold of appearance of clusters at all wavelengths. At 1064, 532, and 355 nm, the production of “heavy” cations as a function of fluence showed a maximum, indicating the participation of competitive effects, whereas saturation is observed at 266 nm. In terms of relative production, the contribution of the “heavy” family to the total cation signal was significantly lower for 266 nm than for the longer wavelengths. Irradiation at 355 nm in the fluence region of 200 mJ/cm² has been identified as the optimum for the generation of large clusters in CdS.     

Energy efficiency of femtosecond laser ablation of refractory metals

We present the results of an experimental study of the ablation energy thresholds and ablated mass for a number of refractory metals (Ti, Zr, Nb, Mo) by femtosecond (τ _0.5 = 45–70 fs) exposed to laser pulses in the ultraviolet — near infrared range (λ = 266, 400, 800 nm) under atmospheric conditions and under vacuum (p ~ 10^–2 Pa). We have analyzed the ablation efficiency (mass yield per unit energy of the acting coherent radiation) and ablation energy thresholds vs. the laser pulse duration and photon energy.     

Laser damage and ablation of differently prepared CaF2(111) surfaces

Ablation thresholds and damage behavior of cleaved and polished CaF₂(111) surfaces produced by single shot irradiation with 248 nm/14 ns laser pulses have been investigated using the photoacoustic mirage technique and scanning electron microscopy. The standard polishing yields an ablation threshold of typically 20 J/cm². When surfaces are polished chemo-mechanically the threshold is raised to 43 J/cm². Polishing by diamond turning leads to intermediate values around 30 J/cm². Cleaved surfaces possess no well-defined damage threshold. The damage topography of conventionally polished surfaces shows ablation of flakes across the laser heated area with cracks along the cleavage planes. In the case of chemo-mechanical polishing only a few cracks appear. Diamond turned surfaces show small optical absorption, but cracks and ablation of tiles. The origin of such different damage behavior is discussed. Presented at the VIII-th Symposium on Surface Physics, Třešt’ Castle, Czech Republic, June 28 – July 2, 1999. This work was funded by the Deutsche Forschungsgemeinschaft, Sonderforschungsbereich 337. One of us (J.S.) acknowledges support from Deutscher Akademischer Austauschdienst and Gottfried Daimler- und Carl Benz-Stiftung.     

Parametric study on femtosecond laser pulse ablation of Au films

Ablation process of 1 kHz rate femtosecond lasers (pulse duration 148 fs, wavelength 775 nm) with Au films on silica substrates has been systemically studied. The single-pulse threshold can be obtained directly. For the multiple pulses the ablation threshold varies with the number of pulses applied to the surface due to the incubation effect. From the plot of accumulated laser fluence N × ?_th(N) and the number of laser pulses N, incubation coefficient of Au film can be obtained (s = 0.765). As the pulse energy is increased, the single pulse ablation rate is increasing following two ablation logarithmic regimes, which can be explained by previous research.     

Surface ablation of lithium tantalate by femtosecond laser

We report measurements of the laser induced breakdown threshold in lithium tantalate with different number of pulses delivered from a chirped pulse amplification Ti: sapphire system. The threshold fluences were determined from the relation between the diameter D² of the ablated area and the laser fluence F₀. The threshold of lithium tantalite under single-shot is found to be 1.84 J/cm², and the avalanche rate was determined to be 1.01 cm²/J by calculation. We found that avalanche dominates the ablation process, while photoionization serves as a free electron provider.     

Shock waves in laser-pulse-irradiated metals

In an earlier paper [1] the temperature as a function of time and distance from the surface of a metal after the application of a laser pulse had been calculated. The assumption was made that only heat conduction is responsible for the dissipation of energy provided that the input fluence of the laser pulse is below the threshold for ablation. In this investigation an estimate for the pressure in the shock wave as a function of time and distance is presented. The assumption mentioned above is valid up to an input fluence of about φ=10 mJ/cm². For larger fluences (but below the ablation threshold) a correction for the dissipation of acoustic energy must be applied. The effect of surface evaporation on T_max and p_max of metals with high melting point is discussed. With fast pulses and/or relatively low velocities of sound, maximum pressures p_max of the shock wave are calculated which are higher than the corresponding stationary values (see (4)). Received: 27 April 2000 / Final version: 6 June 2000 / Accepted: 8 June 2000 / Published online: 13 September 2000     

Measurements of nanoparticle size distribution produced by laser ablation of tungsten and boron-carbide in N2 ambient

Nanoparticles (NPs) were produced by ablating tungsten and boron-carbide (B₄C) target materials in atmospheric pressure nitrogen ambient using ArF excimer laser pulses. The size distributions of the NPs formed during the ablation were monitored—within a 7-133 nm size window—by a condensation particle counter connected to a differential mobility analyzer. The laser repetition rate was varied between 1-50 Hz, and the fluence was systematically changed in the range of 0.5-15 J/cm², for both materials, allowing a comparative study in an extended laser parameter regime. The multishot ablation threshold (Φ_th) of B₄C was determined to be ∼1.9 J/cm² for the laser used (ArF excimer, λ = 193 nm). Similarly to earlier studies, it was shown that the size distributions consist of mainly small nanoparticles (<∼20 nm) attributed to a non-thermal ablation mechanism below Φ_th. An additional broad peak appears (between 20 and 40 nm) above Φ_th as a consequence of the thermally induced macroscopic ablation. Chemical composition of deposited polydisperse nanoparticles was studied by X-ray photoelectron spectroscopy showing nitrogen incorporation into the boron-carbide.     

Influence of storage time on laser cleaning of SiO<Subscript>2</Subscript> on Si

The influence of the ‘storage time’ τ_s on the threshold fluence φ_cl and the efficiency in dry laser cleaning is investigated. τ_s denotes the time between the deposition of particles and the cleaning. As a model system we employed silica spheres with diameters of 500 nm and 1500 nm on commercial silicon wafers and single-pulse KrF excimer laser radiation (τ_FWHM=28 ns). For the 1500-nm silica spheres, φ_cl was found to increase from about 65 mJ/cm² to 125 mJ/cm² for storage times of 4 h and 362 h, respectively. For 500-nm silica spheres the increase in the threshold fluence was less than 20% for storage times up to 386 h. Received: 12 July 2002 / Accepted: 12 July 2002 / Published online: 29 January 2003 RID="*" ID="*"Corresponding author. E-mail:dieter.baeurle@jku.at     

Femtosecond pulsed laser ablation of diamond-like carbon films on silicon

Femtosecond pulsed laser ablation (τ = 120 fs, λ = 800 nm, repetition rate = 1 kHz) of thin diamond-like carbon (DLC) films on silicon was conducted in air using a direct focusing technique for estimating ablation threshold and investigating the influence of ablation parameter on the morphological features of ablated regions. The single-pulse ablation threshold estimated by two different methods were ?_th(1) = 2.43 and 2.51 J/cm². The morphological changes were evaluated by means of scanning electron microscopy. A comparison with picosecond pulsed laser ablation shows lower threshold and reduced collateral thermal damage.     

Dynamic behavior of photoablation products of corneal tissue in the mid-IR: a study with FELIX

2 . Dynamic parameters such as the extension of the ablation cloud, the initial velocity and momentum of the ablated particles as well as the ablation threshold, the ablated mass, and the particle size were investigated. The ablation plume was made visible with a stroboscopic technique. For a fluence of 3.1 J/cm² the average initial velocity of the ejected particles was deduced from the extension of the plume to range from 120–400 m/s. Measurements of the recoil momentum using a sensitive pendulum led to values between 0.5 and 2.0 mm g/s. All measured properties were related to the spectroscopically determined absorption coefficient of cornea α_cornea. Where absorption due to proteins is high (at λ=6.2 and 6.5 μm), ablated mass, velocity and recoil momentum behave according to α_cornea. For the first time, variations of the ablation plume from pulse to pulse were observed. Those, as well as the particle size, not only depend on the absorption coefficient, but also on the predominant absorber. Received: 4 November 1997/Revised version: 7 September 1998     

Dynamics of ions produced by laser ablation of ceramic Al<Subscript>2</Subscript>O<Subscript>3</Subscript> and Al at 193 nm

We study the dynamics of ions produced upon ablation of Al and ceramic Al₂O₃ targets using nanosecond laser pulses at 193 nm (6.4 eV) as a function of the laser fluence from threshold up to 12 J cm⁻². An electrical (Langmuir) probe located at 40 mm from the target surface has been used for determining the ion yield and calculating the kinetic energy distributions. The results for both targets show the existence of a significant amount of ions having kinetic energies >200 eV (≈20% around threshold fluence), and kinetic energies are up to >1.5 keV. The results are related with the existence of direct photonionization processes caused by the photon energy of the laser being higher than the ionization potential of Al (5.98 eV). Comparison of the ion yield when ablating the two types of targets for fluences above threshold to data reported in the literature suggests that the magnitude of the yield and its threshold are parameters depending on the thermal properties of the target rather than on the laser wavelength. Around threshold, the different behavior of ion yield when ablating Al and Al₂O₃ targets suggests that the threshold for neutral aluminium and ion species in the case of ablation of the Al₂O₃ target must be similar.     

Short-pulse UV laser ablation of solid and liquid metals: indium

2 to 2.5 mJ/cm² when a 0.5 ps pulse is used instead of a 15 ns laser pulse. Measurements on liquid indium show a different behavior. With 15 ns laser pulses the threshold fluence is lowered by a factor of ∼3 from 100 mJ/cm² for solid indium to 30 mJ/cm² for liquid indium. In contrast, measurements with 0.5 ps laser pulses do not show any change in the ablation threshold and are independent of the phase of the metal at 2.5 mJ/cm². This behavior could be explained by thermal diffusion and heat conduction during the laser pulse and demonstrates in an independent way the energy lost into the material when long laser pulses are applied. Time-of-flight measurements to investigate the underlying ablation mechanism show thermal behavior of the ablated indium atoms for both ps and ns ablation and can be fitted to Maxwell-Boltzmann distributions. Received: 2 December 1996/Accepted: 11 December 1996     

Selective removal and patterning of a Co/Cu/Co trilayer created by femtosecond laser processing

The selective removal and patterning of a typical pseudo-spin-valve structure, consisting of a Co(20 nm)/ Cu(6 nm)/Co(3 nm) trilayer, by femtosecond laser has been examined in terms of irradiation parameters and layer structure. Ablation thresholds of the individual Co and Cu thin films and the SiO₂/Si substrate have been measured for single-shot irradiation with a 200 femtosecond (fs) laser pulses of a Ti:sapphire laser operating at 775 nm. Ablation of the entire trilayer structure was characterized by a sequential removal of the layers at a threshold level of fluence of 0.28 J/cm². Atomic Force Microscopy, optical microscopy, profilometry and Sputtered Neutral Mass Spectroscopy were employed to characterize the laser-induced single-shot laser selective removal and patterned areas. As a result, two phenomena were found to characterize the laser process: (i) selective removal of the Co and Cu layer due to the change of the laser fluence and (ii) regular pillars’ area of Co/Cu/Co could be achieved in a regular manner with the lowest pillar width size of 1.5 μm. Ablation through the layers was accompanied by the formation of bulges at the edges of the pillars, which was the biggest inconvenience in lowering the pillar size through the femtosecond laser process.     

Picosecond laser ablation of nickel-based superalloy C263

Picosecond laser (10.4 ps, 1064 nm) ablation of the nickel-based superalloy C263 is investigated at different pulse repetition rates (5, 10, 20, and 50 kHz). The two ablation regimes corresponding to ablation dominated by the optical penetration depth at low fluences and of the electron thermal diffusion length at high fluences are clearly identified from the change of the surface morphology of single pulse ablated craters (dimples) with fluence. The two corresponding thresholds were measured as F _th(D1)¹=0.68±0.02 J/cm² and F _th(D2)¹=2.64±0.27 J/cm² from data of the crater diameters D _1,2 versus peak fluence. The surface morphology of macroscopic areas processed with a scanning laser beam at different fluences is characterised by ripples at low fluences. As the fluence increases, randomly distributed areas among the ripples are formed which appear featureless due to melting and joining of the ripples while at high fluences the whole irradiated surface becomes grainy due to melting, splashing of the melt and subsequent resolidification. The throughput of ablation becomes maximal when machining at high pulse repetition rates and with a relatively low fluence, while at the same time the surface roughness is kept low.     

Improvement of the pinning properties of (Bi/Pb)-2223 textured ceramics by columnar defects introduced by 6 GeV Pb ions

Pinning properties of (Bi/Pb)-2223 textured ceramics have been improved by 6 GeV Pb ions irradiation. Two samples were irradiated at fluencesφ _t=5 × 10¹⁰ ions/cm² and 2 × 10¹¹ ions/cm², respectively. The magnetic irreversibility is clearly improved in the intermediate range of temperature: (30–35) K<T<60 K for magnetic fields lower than the “fluence equivalent field”B _φ =φ _t.φ ₀. Moreover the irreversibility line is shifted towards higher fields. The results reported here show that the introduction of columnar defects or other extended defects is a route to improve the screening properties of tubes or cans based on (Bi/Pb)-2223 material and operating in liquid nitrogen.     

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.