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     

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.     

Femtosecond-pulse laser ablation of human corneas

A femtosecond pulse laser in the visible spectral region shows promise as a potentially new powerful corneal sculpting tool. It combines the clinical and technical advantages of visible wavelengths with the high ablation quality observed with nanosecond-pulse excimer lasers at 193 nm. A femtosecond and a nanosecond dye laser with pulse durations of 300 fs and 7 ns, and centre wavelengths at 615 nm and 600 nm, respectively, both focused to an area of the order of 10^–5 cm², have been applied to human corneal ablation. Nanosecond laser pulses caused substantial tissue disruption within a 30–100 m range from the excision edge at all fluences above the ablation threshold of F _th60 J cm^–2 (I _th9 GW cm^–2). Completely different excisions are produced by the femtosecond-pulse laser: high quality ablations of the Bowman membrane and the stroma tissue characterised by damage zones of less than 0.5 m were observed at all fluences above ablation threshold of F _th1 J cm^–2 or I _th3 TW cm^–2 (3×10¹² W cm^–2). The transparent cornea material can be forced to absorb ultrashort pulses of extremely high intensity. The fs laser generates its own absorption by a multiphoton absorption process.     

Single-shot ablation threshold of chromium using UV femtosecond laser pulses

Single-shot ablation threshold for thin chromium film was studied using 266 nm, femtosecond laser pulses. Chromium is a useful material in the nanotechnology industry and information on ablation threshold using UV femtosecond pulses would help in precise micromachining of the material. The ablation threshold was determined by measuring the ablation crater diameters as a function of incident laser pulse energy. Absorption of 266 nm light on the chromium film was also measured under our experimental conditions, and the absorbed energy single-shot ablation threshold fluence was \(46 \pm 5\)  mJ/cm². The experimental ablation threshold fluence value was compared to time-dependent heat flow calculations based on the two temperature model for ultrafast laser pulses. The model predicts a value of 31.6 mJ/cm² which is qualitatively consistent with the experimentally obtained value, given the simplicity of the model.     

High-energy long-pulse Nd:YAG picosecond laser

A long train of actively mode-locked pulses is obtained from a negative feedback controlled Nd:YAG laser. The 70s pulse train contains up to 0.1 J energy and the duration of the picosecond pulses is 120 ps. The laser is operated at a repetition rate of 20 Hz. ActiveQ-control of the cavity generates a short pulse train of duration 50 to 70 ns. An excellent peak-to-background intensity ratio of the correlation function for the picosecond pulses in the train of 5×10³ is reported.     

Ablation of polyimide (Kapton™) films by pulsed (ns) ultraviolet and infrared (9.17 μm) lasers

Ablation of the surface of a polyimide (Kapton) film by single pulses of 248 nm or 308 nm radiation (20 ns) or 9.17 m laser radiation (170 ns) was studied by photographing the emergence of the blast wave and the plume by a pulse (<1 ns; 596 nm) of visible laser light. The dynamics of the blast wave was similar in the ultraviolet and in the infrared but the composition of the plume was obviously different. A mass of opaque solid material was ejected for as long as 2.6 s following the IR pulse in contrast to the minute amount of solids that are seen in the ablation by UV laser pulses of ns duration. UV laser pulses of 50–400 s duration interact with polyimide surfaces in a manner that is similar to IR laser pulses of ns duration or longer. Chemical analysis of the ablation products that are obtained under various conditions of ablation when compared to the known modes of thermal degradation of polyimide show that the reaction is a thermal process when IR laser pulses or UV laser pulses of long (>10 s) duration are employed. Ablation by ns UV laser pulses differs fundamentally in the chemistry of the products from all of the cases mentioned above.     

Nanosecond and femtosecond excimer-laser ablation of oxide ceramics

The uv laser-ablation behavior of various oxide ceramics (Al₂O₃, MgO, ZrO₂) has been studied using different wavelengths (248 nm, 308 nm) and pulse durations (30 ns, 500 fs). Time-resolved absorption measurements of the sample and the ablation plume during ablation were performed.Using sub-ps pulses the ablation threshold fluence is generally lower than for ns pulses; the ablation rate is higher in the whole investigated fluence range up to 20 J/cm².The study of the morphology of the ablation structures and the results of the absorption experiments lead to the conclusion that different ablation mechanisms are involved. Using ns pulses plasma mediated ablation is dominating, whereas in the fs case the process is controlled by multi-photon absorption enabling microstructuring of the material.     

Prepulse dependence ofJ=0−1 lasing at 32.6 nm in neon-like titanium

The dependence of the intensity of the 3p—3s,J = 0–1 lasing line at 32.6 nm in neon-like titanium on the prepulse level has been investigated experimentally. Titanium slabs were irradiated with 1.315 µm/450 ps pulses from the Asterix IV iodine laser using a defined prepulse of 5.2 ns before the main pulse. It is found that for pump energies close to the minimum energy for which lasing is observed, a prepulse level of order 0.5% gives the highest XUV laser intensity, whereas a higher prepulse level, of order 10% and more, is required for optimum XUV lasing far above the threshold. For a 2.7 cm long titanium target lasing was observed down to a pump irradiance of 2.5 TW/cm² (50 J/450 ps) for the 0.5% prepulse.     

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.     

Femtosecond uv excimer laser ablation

Experiments on the ablation of polymethylmethacrylate (PMMA) with 300 fs uv excimer laser pulses at 248 nm are reported for the first time. With these ultrashort pulses, ablation can be done at fluences up to five times lower than the threshold fluence for 16 ns ablation of PMMA, and the surface morphology is improved, also for several other materials. A model for ablation is proposed, assuming a non-constant absorption coefficient _eff depending on the degree of incubation of the irradiated material and the intensity of the incoming excimer laser pulse. The agreement between our model and our experimental observations is excellent for 16 ns excimer laser pulses, also predicting perfectly the shape of a pulse transmitted through a thin PMMA sample under high fluence irradiation. Qualitative agreement for 300 fs excimer laser pulses is obtained so far.     

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.     

Comparison of simulated X-ray conversion efficiency of laser produced iron plasma with experimental results

X-ray resonance lines between 11 Å and 17 Å emitted from iron plasmas created by a modest KrF laser have been simulated by modifying the atomic and hydrodynamic code EHYBRID. Free–free and free–bound emission from the Si-, Al-, Mg-, Na-, Ne- and F-like ions is calculated in the simulation. In the original experiments, a KrF laser (249 nm wavelength) with focused irradiances between 1×10¹² W/cm² and 1×10¹⁵ W/cm² was focused on iron targets. The laser pulse duration was varied between 10 ps and 20 ns. We have calculated X-ray conversion efficiencies to be, for example, 0.5% over 2 sr for 2×10¹³ W/cm² and 20 ns pulse duration, in good agreement with experimental measurements. The simulation of X-ray emission is also presented for an experiment where a train of eight 7 ps KrF laser pulses is incident onto an iron target. PACS 52.50.Jm; 52.38.Ph; 52.65.Kj; 52.30.Ex; 32.30.Rj     

Dynamics of phase transitions induced by femtosecond laser pulse irradiation of indium phosphide

The structural transformation dynamics of single-crystalline indium phosphide (InP) irradiated with 150 fs laser pulses at 800 nm has been investigated by means of time-resolved reflectivity measurements covering a time window from 150 fs up to 500 ns. The results obtained show that for fluences above a threshold of 0.16 J/cm² thermal melting of the material occurs on the timescale of 1–2 ps. The evolution of the reflectivity on a longer timescale reveals the reflectivity of the liquid phase and shows resolidification times typically around 10–30 ns after which an amorphous layer several tens of nanometers thick is formed on the surface. This amorphous layer significantly alters the optical properties of the surface and finally leads to a reduced ablation threshold for subsequent laser pulses. Single-pulse ablation at higher fluences (>0.23 J/cm²) is preceded by an ultrafast phase transition (non-thermal melting) occurring within 400 fs after the arrival of the pulse to the surface. PACS 79.20.Ds; 78.47.+p; 64.70.-p     

Direct observation of laser-induced crystallization of a-C:H films

The post-growth modification of diamond-like amorphous hydrogenated carbon a-C:H films by laser treatment has been studied by transmission electron microscopy and Raman spectroscopy. a-C:H films grown on Si substrates by benzene decomposition in a rf glow discharge were irradiated with 15 ns pulses of a KrF-excimer laser with fluences in the range of E=50–700 mJ/cm². At fluences below 100 mJ/cm² an increase in the number of graphitic clusters and in their ordering was evidenced from Raman spectra, while the film structure remained amorphous according to electron microscopy and electron diffraction observations. At higher fluences the appearance of diamond particles of 2–7 nm size, embedded into the lower crystallized graphitic matrix, was observed and simultaneously a progressive growth of graphite nanocrystals with dimensions from 2 nm to 4 nm was deduced from Raman measurements. The maximum thickness of the crystallized surface layer (400 nm) and the degree of laser annealing are limited by the film ablation which starts at E>250 mJ/cm². The laser-treated areas lose their chemical inertness. In particular, chemical etching in chromium acid becomes possible, which may be used for patterning the highly inert carbon films.     

Excimer-laser-induced permanent electrical conductivity in solid C60 films

After being irradiated in air by a XeCI (308 nm) excimer laser, the electrical conductivity of solid thin-film C₆₀ has been improved by more than six orders of magnitudes. The products resulting from laser irradiation of C₆₀ films have been investigated by Raman scattering and the onset of conductivity can be attributed to laser-induced oxygenation and disintegration of the fullerene. Irradiated by 40 ns laser pulses with different fluence, products with different microstructure were observed. At lower fluence, the Raman features of microcrystalline graphite and fullerene polymer were observed. At a fluence just below the ablation threshold (36 mJ/cm²), the fullerene molecules in the film were disintegrated completely and transformed to amorphous graphite.     

All-optical ion generation for ion trap loading

We have investigated the all-optical generation of ions by photo-ionisation of atoms generated by pulsed laser ablation. A direct comparison between a resistively heated oven source and pulsed laser ablation is reported. Pulsed laser ablation with 10 ns Nd:YAG laser pulses is shown to produce large calcium flux, corresponding to atomic beams produced with oven temperatures greater than 650 K. For an equivalent atomic flux, pulsed laser ablation is shown to produce a thermal load more than one order of magnitude smaller than the oven source. The atomic beam distributions obey Maxwell–Boltzmann statistics with most probable speeds corresponding to temperatures greater than 2200 K. Below a threshold pulse fluence between 280 mJ/cm² and 330 mJ/cm², the atomic beam is composed exclusively of ground-state atoms. For higher fluences ions and excited atoms are generated.     

KrF excimer laser processing of thick diamond-like carbon films

Ablation characteristics of a commercially available diamond-like carbon (DLC) film (the EVERSCAN^TM bar code scanner window; Diamonex Division of Morgan Advanced Ceramics Inc.) in the 0–7 Jcm^-2 fluence window are reported. Glass pieces covered with 6 m thick DLC coating are ablated by 22 ns pulses of a KrF excimer laser in medium vacuum (10^-1 Pa), and in Ar and O₂ atmospheres of 10⁵ Pa. The ablation depth increases strictly linearly with an increasing number of pulses, independently of the atmosphere and the applied fluence. The threshold lies at 0.13 Jcm^-2 and is independent of the atmosphere. While above 1 Jcm^-2 the ablation rate vs. fluence plots recorded in different atmospheres coincide within experimental error, processing under vacuum between 0.5 and 1 Jcm^-2 results in significantly higher ablation rate values. Ablation rates exceeding 100 nm/pulse above 1 Jcm^-2 ensure extremely efficient machining over extended areas even at relatively low fluences. Identical characteristics in Ar and O₂ atmospheres suggest that solely physical (ablative) processes contribute to material removal. PACS 42.62.-b; 61.80.Ba; 68.35.Rh; 81.05.Uw     

Efficient amplification of sub-picosecond pulses of a non-CW dye laser

Efficient amplification in a dye laser amplifier is investigated theoretically and experimentally. A five-level rate equation approach is considered including rotational relaxation of the dye molecules. The effects of the pump pulse duration and of the parameters of the input pulse are discussed. The results are compared with experimental data for 0.5 ps pulses of a pulsed dye laser. Conversion efficiencies >10% are achieved for a single pass amplifier using Nd:YAG pump pulses of 2 ns while an effective fluorescence lifetime of 1.7±0.2 ns is determined for the gain medium rhodamine 6G. The triple pass amplifier stage of the laser system achieves an energy conversion of 4% with 40 J output pulses.     

Mid-infrared nonlinear phenomena in polycrystalline semiconductors

We have studied second-harmonic generation by 30 ps and 70 ns 10 m CO₂ laser pulses in nonlinear polycrystalline ZnSe, CdTe and GaAs samples. Second-harmonic generation in these materials can limit the amplification of high-power CO₂-laser pulses in amplifier chains sealed with these polycrystalline IR-transmission materials. On the other hand, we now demonstrate for the first time that these materials are suited as nonliner elements for autocorrelation measurements on short infrared laser pulses. For such pulse-width measurements polycrystalline materials have an advantage over single crystals, e.g. GaAs, because they are insensitive to misalignement. Furthermore, these polycrystalline optical elements are easier and cheaper to manufacture than single crystal devices. With such polycrystalline materials we were able to realize reliable autocorrelation measurements of 30–300 ps 10 m optical-free-induction-decay (OFID) laser pulses.     

Generation of picosecond and subpicosecond light pulses with saturable absorbers

Single light pulses, generated by a mode-locked Nd-glass laser, were shortened with saturable absorbers of low initial transmissionT ₀. The pulse duration was reduced from 8 to 2.6 ps after a single pass through a dye cell ofT ₀=10^–7. Light pulses as short as 0.5 ps were observed after five transits through an absorberamplifier system. Detailed calculations of the stationary and the transient situation (with respect to the dye relaxation time) are presented to demonstrate optimum conditions for the pulse shortening.