Selective ablation of thin SiO<Subscript>2</Subscript> layers on silicon substrates by femto- and picosecond laser pulses

The selective ablation of thin (∼100 nm) SiO₂ layers from silicon wafers has been investigated by applying ultra-short laser pulses at a wavelength of 800 nm with pulse durations in the range from 50 to 2000 fs. We found a strong, monotonic decrease of the laser fluence needed for complete ablation of the dielectric layer with decreasing pulse duration. The threshold fluence for 100% ablation probability decreased from 750 mJ/cm² at 2 ps to 480 mJ/cm² at 50 fs. Significant corruption of the opened Si surface has been observed above ∼1200 mJ/cm², independent of pulse duration. By a detailed analysis of the experimental series the values for melting and breaking thresholds are obtained; the physical mechanisms responsible for the significant dependence on the laser pulse duration are discussed.     

Parametric oscillation of high-power 3-THz pulse by synchronously pumped ZnGeP<Subscript>2</Subscript> crystal: Computer simulation

Possible parametric oscillation of 3-THz pulse at synchronous pumping of the ZnGeP₂ crystal by a train of short second-harmonic pulses from the CO₂ laser has been analyzed. Calculation shows that at changing laser pulse duration τ between 4 and 500 ps and correspondingly pumping energy density (0.5–3.5 J cm⁻²) THz pulse peak power varies from 3 to 70MW with maximum at τ =9 ps.     

A comparative study of the ionic keV X-ray line emission from plasma produced by the femtosecond,picosecond and nanosecond duration laser pulses

We report here an experimental study of the ionic keV X-ray line emission from magnesium plasma produced by laser pulses of three widely different pulse durations (FWHM) of 45 fs, 25 ps and 3 ns, at a constant laser fluence of ∼1.5 × 10⁴ J cm^− 2. It is observed that the X-ray yield of the resonance lines from the higher ionization states such as H- and He-like ions decreases on decreasing the laser pulse duration, even though the peak laser intensities of 3.5 × 10¹⁷ W cm^− 2 for the 45 fs pulses and 6.2 × 10¹⁴ W cm^− 2 for the 25 ps pulses are much higher than 5 × 10¹² W cm^− 2 for the 3 ns laser pulse. The results were explained in terms of the ionization equilibrium time for different ionization states in the heated plasma. The study can be useful to make optimum choice of the laser pulse duration to produce short pulse intense X-ray line emission from the plasma and to get the knowledge of the degree of ionization in the plasma.     

The role of electron-phonon coupling in femtosecond laser damage of metals

Femtosecond laser pulses were applied to study the energy deposition depth and transfer to the lattice for Au, Ni, and Mo films of varying thickness. The onset of melting, defined here as damage threshold, was detected by measuring changes in the scattering, reflection and transmission of the incident light. Experiments were done in multi-shot mode and single-shot threshold fluences were extracted by taking incubation into account. Since melting requires a well-defined energy density, we found the threshold depends on the film thickness whenever this is smaller than the range of electronic energy transport. The dependence of the threshold fluence on the pulse length and film thickness can be well described by the two-temperature model, proving that laser damage in metals is a purely thermal process even for femtosecond pulses. The importance of electron-phonon coupling is reflected by the great difference in electron diffusion depths of noble and transition metals.     

Femtosecond laser ablation of silver foil with single and double pulses

The average ablation depth per pulse of silver foil by 130 fs laser pulses has been measured in vacuum over a range of three orders of magnitude of pulse fluence up to 900 J cm⁻². In addition, double pulses with separations up to 3.4 ns have been used to probe time scales of relevance for femtosecond ablation. The double pulse ablation depth, when each pulse fluence is 0.7 J cm⁻², falls to that of a single pulse as the pulse separation is increased from 0 ps to 700 ps. This time scale decreases to only 4 ps as the fluence is increased to 11 J cm⁻². It then jumps to 500 ps across a transition fluence where the slope of the ablation depth versus logarithmic fluence characteristic changes abruptly to a higher value. In addition, for pulse separations near 1000 ps, the second pulse can cause re-deposition of ejecta from the first pulse resulting in a double pulse ablation depth only 40% that of the first pulse alone. This has important implications for the interpretation of double pulse femto-LIBS intensities. Our results suggest that the optical properties of nano or mesoparticles play a significant role in double pulse ablation with large pulse separations.     

Impact of the lasr wavelength and fluence on the ablation rate of aluminium

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.      

Nonlinear energy absorption of femtosecond laser pulses in noble metals

We use calorimetry to determine the energy absorption of femtosecond (fs) laser pulses as a function of incident fluence for Ag, Ag alloys (Ag–Cu and Ag–Pt), and Pt. At low fluences, the measured absorption agrees well with reflectivity data derived from ellipsometry measurements. For Ag and Ag–Cu, the absorbed energy increases nonlinearly with the incident fluence for fluences larger than approximately half of the melting threshold. Near this threshold, the absorption increases by a factor of 3–4. Similar nonlinear absorption is not observed in Pt or Ag–Pt. We propose that the nonlinear absorption is caused by the excitation of d-band electrons below the Fermi surface. For pulse widths longer than 850 fs, the observed nonlinear absorption in Ag diminishes, indicating that diffusive transport and not ballistic transport is the major mechanism of cooling at this excitation level.     

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.     

Incubation effect and its influence on laser patterning of ITO thin film

Results are presented on the surface damage thresholds of ITO thin films induced by single- and multi-pulse laser irradiation at a pulse duration of 10 ps and a wavelength of 1064 nm. For multi-pulse ablation the incubation effect results in a reduction of the damage threshold, especially apparent at low pulse numbers and very small film thicknesses. The incubation effect attributes to the accumulation of defect sites and/or the storage of thermal stress-strain energy induced by the incident laser pulses. An incubation coefficient of S=0.82 has been obtained which is independent on the film thickness in the range of 10–100 nm. In practical applications, the incubation effect determines the laser patterning structure of ITO films while increasing the pulse overlapping rate. The width of the patterned line can be predicted by the proposed model involving the laser fluence, the overlapping rate and the incubation coefficient.     

Femtosecond laser ablation of silicon–modification thresholds and morphology

We investigated the initial modification and ablation of crystalline silicon with single and multiple Ti:sapphire laser pulses of 5 to 400 fs duration. In accordance with earlier established models, we found the phenomena amorphization, melting, re-crystallization, nucleated vaporization, and ablation to occur with increasing laser fluence down to the shortest pulse durations. We noticed new morphological features (bubbles) as well as familiar ones (ripples, columns). A nearly constant ablation threshold fluence on the order of 0.2 J/cm² for all pulse durations and multiple-pulse irradiation was observed. For a duration of ≈100 fs, significant incubation can be observed, whereas for 5 fs pulses, the ablation threshold does not depend on the pulse number within the experimental error. For micromachining of silicon, a pulse duration of less than 500 fs is not advantageous. Received: 4 December 2000 / Revised version: 29 March 2001 / Published online: 20 June 2001     

Effect of melting on the excitation of surface acoustic wave pulses by UV nanosecond laser pulses in silicon

The influence of melting on the excitation of Surface Acoustic Wave (SAW) pulses in silicon is studied both theoretically and experimentally. The developed theory of Rayleigh-type SAW laser-induced thermoelastic excitation in a structure composed of a liquid layer on a solid substrate predicts that the SAW is predominantly generated in the solid phase due to the absence of shear rigidity in a liquid. The characteristic changes in the SAW pulse shape as well as the saturation and even the decrease of the SAW pulse amplitude observed above the melting threshold are explained theoretically to be a result of the decrease of the heat flux into the solid phase as well as due to the decrease of the volume of the solid phase caused by melting. Although the heat flux into the solid phase is decreased both as a consequence of the reflectivity increase and the additional energy losses (latent heat of melting) at the phase transition, it is demonstrated that the influence of reflectivity changes on the SAW pulse is negligible in comparison with the effect of melt-front motion. For laser pulses of 7 ns duration at 355 nm, the threshold value of laser fluence for meltingF _m=0.23±0.04 J/cm² and for the ablationF _a=1.3±0.2 J/cm² were determined experimentally as the points of characteristic changes in the observed SAW pulses.     

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     

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.     

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.     

Ripples and grain formation in GaAs surfaces exposed to ultrashort laser pulses

The damage morphology of GaAs1 0 0 single crystal following femtosecond laser (wavelength 806 nm, pulse duration 110 fs, prf 10 Hz) excitation was studied as a function of laser fluence and number of pulses. The threshold value for damage to occur in a GaAs surface in the present experiment was 1.3×10¹⁴ W/cm² for a single pulse. The cooling rate for threshold fluence was calculated as 2.22×10¹⁴ °C/s. The damage occurred in the form of surface removal. Ripples and grains were formed in the removed surface. At higher fluences micron depth pits were also formed. The damage morphology was explained with the help of Boson-condensation hypothesis.     

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.     

888 nm pumped 1342 nm Nd:YVO<Subscript>4</Subscript> oscillator Kerr-lens mode-locked using cascaded second-order nonlinearities

We report on a parametric Kerr-lens mode-locked 888 nm pumped Nd:YVO₄ 1342 nm oscillator using cascaded second-order nonlinearities in LBO. Stable ps-pulse-operation was achieved. For an output coupling of T=25% high average output power of 6.5 W, emitting Fourier-limited pulses with a duration of 10 ps was reached. By changing the output coupling to T=10%, we achieved much shorter pulses with a pulse duration of 4 ps for less lower average power of 4.8 W. The beam was diffraction limited with an M ² parameter better than <1.05.     

Laser acceleration of electrons in a thin metal film

A mechanism acceleration of electrons to relativistic velocities in a thin metal film irradiated with ultrashort (τ _L ≤1 ps) high-power (I>¹⁶ W/cm²) laser pulses is proposed. The acceleration is due to a resonance action of the nonuniform field on a portion of the electrons, viz., those which oscillate in the direction transverse to the film with a frequency close to the frequency of the field. Pis’ma Zh. éksp. Teor. Fiz. 66, No. 1, 8–12 (10 July 1997)