Nanospallation induced by an ultrashort laser pulse

A femtosecond laser pulse with power density of 10¹³ to 10¹⁴ W/cm² incident on a metal target causes ablation and ejection of the surface layer. The ejected laser plume has a complicated structure. At the leading front of the plume, there is a spall layer where the material is in a molten state. The spall layer is a remarkable part of the plume in that the liquid-phase density does not decrease with time elapsed. This paper reports theoretical and experimental studies of the formation, structure, and ejection of the laser plume. The results of molecular dynamics simulations and a theoretical survey of plume structure based on these results are presented. It is shown that the plume has no spall layer when the pulse fluence exceeds an evaporation threshold F _ev. As the fluence increases from the ablation threshold F _a to F _ev, the spall-layer thickness for gold decreases from 100 nm to a few lattice constants. Experimental results support theoretical calculations. Microinterferometry combined with a pump-probe technique is used to obtain new quantitative data on spallation dynamics for gold. The ablation threshold is evaluated, the characteristic crater shape and depth are determined, and the evaporation threshold is estimated.     

Molecular dynamics simulation of femtosecond ablation and spallation with different interatomic potentials

Fast heating of target material by femtosecond laser pulse (fsLP) with duration τ_L∼40-100 fs results in the formation of thermomechanically stressed state. Its unloading may cause frontal cavitation of subsurface layer at a depth of 50 nm for Al and 100 nm for Au. The compression wave propagating deep into material hits the rear-side of the target with the formation of rarefaction wave. The last may produce cracks and rear-side spallation. Results of MD simulations of ablation and spallation of Al and Au metals under action fsLP are presented. It is shown that the used EAM potentials (Mishin et al. and our new one) predict the different ablation and spallation thresholds on absorbed fluence in Al: ablation F_a=60{65} mJ/cm²and spallation F_s=120{190} mJ/cm², where numbers in brackets { } show the corresponding values for Mishin potential. The strain rate in spallation zone was 4.3×10⁹ 1/s at spallation threshold. Simulated spall strength of Al is 7.4{8.7} GPa, that is noticeably less than 10.3{14} GPa obtained from acoustic approximation with the use of velocity pullback on velocity profile of free rear surface. The ablation threshold F_a≈120 mJ/cm² and crater depth of 110 nm are obtained in MD simulations of gold with the new EAM potential. They agree well with experiment.     

Laser fluence, repetition rate and pulse duration effects on paint ablation

The efficiency (mm³/(J pulse)) of laser ablation of paint was investigated with nanosecond pulsed Nd:YAG lasers (λ = 532 nm) as a function of the following laser beam parameters: pulse repetition rate (1-10,000 Hz), laser fluence (0.1-5 J/cm²) and pulse duration (5 ns and 100 ns). In our study, the best ablation efficiency (η ≅ 0.3 mm³/J) was obtained with the highest repetition rate (10 kHz) at the fluence F = 1.5 J/cm². This ablation efficiency can be associated with heat accumulation at high repetition rate, which leads to the ablation threshold decrease. Despite the low thermal diffusivity and the low optical absorption of the paint (thermal confinement regime), the ablation threshold fluence was found to depend on the pulse duration. At high laser fluence, the ablation efficiency was lower for 5 ns pulse duration than for the one of 100 ns. This difference in efficiency is probably due to a high absorption of the laser beam by the ejected matter or the plasma at high laser intensity. Accumulation of particles at high repetition rate laser ablation and surface shielding was studied by high speed imaging.     

Model for laser-induced thermal degradation and ablation of polymers

Ablation of organic polymers is described on the basis of photothermal bond breaking within the bulk material. Here, we assume a first-order chemical reaction, which can be described by an Arrhenius law. Ablation starts when the density of broken bonds at the surface reaches a certain critical value. In order to understand the ablation behavior near the threshold fluence, φ_th, non-stationary regimes must be considered. The present treatment reveals several qualitative differences with respect to models that treat ablation as a surface process: (i) Ablation starts sharply with a front velocity that has its maximum value just after the onset. (ii) The transition to the quasi-stationary ablation regime is faster. (iii) Near threshold, the ablated depth h has a square-root dependence on laser fluence, i.e., h∝(φ-φ_th)^1/2. The ablation velocity is very high even near φ_th. (iv) With φ≈φ_th ablation starts well after the laser pulse. (v) The depletion of species is responsible for the Arrhenius tail observed with fluences φ≤φ_th. (vi) Residual modification of material has maximum near the threshold. (vii) Stationary regimes of ablation demonstrate change of effective activation energy with laser intensity. The model calculations are applied to Polyimide (Kapton^TM H). Here, differences in single-pulse ablated depth determined from mass loss and profilometry should be about 10 nm. Received: 16 February 1999 / Accepted: 18 February 1999 / Published online: 28 April 1999     

Influence of laser fluence and irradiation timing of F2 laser on ablation properties of fused silica in F2-KrF excimer laser multi-wavelength excitation process

A collinear irradiation system of F₂ and KrF excimer lasers for high-quality and high-efficiency ablation of hard materials by the F₂ and KrF excimer lasers’ multi-wavelength excitation process has been developed. This system achieves well-defined micropatterning of fused silica with little thermal influence and little debris deposition. In addition, the dependence of ablation rate on various conditions such as laser fluence, irradiation timing of each laser beam, and pulse number is examined to investigate the role of the F₂ laser in this process. The multi-wavelength excitation effect is strongly affected by the irradiation timing, and an extremely high ablation rate of over 30 nm/pulse is obtained between -10 ns and 10 ns of the delay time of F₂ laser irradiation. The KrF excimer laser ablation threshold decreases and its effective absorption coefficient increases with increasing F₂ laser fluence. Moreover, the ablation rate shows a linear increase with the logarithm of KrF excimer laser fluence when the F₂ laser is simultaneously irradiated, while single KrF excimer laser ablation shows a nonlinear increase. The ablation mechanism is discussed based on these results. Received: 16 July 2001 / Accepted: 27 July 2001 / Published online: 2 October 2001     

Self-organization of thin metal films by irradiation with nanosecond laser pulses

Modifications in thin metal films under intensive laser irradiation were studied. Gold, silver, copper, chromium and aluminum films with the thickness of 100 nm were deposited on the glass substrate. Back-side irradiation through the substrate with a burst of nanosecond pulses tightly focused to a line was applied. The film removal threshold with a single pulse F_th was estimated for every material and laser fluence was kept above it in the range of 1.5-3 F_th during experiments. Diverse behavior of the films depending on the metal, the shift between pulses and laser fluence was observed. In chromium, the regular structures were developed in a quite wide range of processing parameters. In gold, three kinds of ripples were observed: transverse (similar to ripples in chromium), longitudinal and a structure of ripples oriented at 60° to each other. The combination of physical properties facilitated the regular assembly of the molten metal in chromium and to some extent in gold.     

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.     

Thresholds for front-side ablation and rear-side spallation of metal foil irradiated by femtosecond laser pulse

The mechanical action of laser exposure on a foil may result in the ablation of irradiated front layer and the rear-side spallation. The dynamics of an Al foil is studied by means of two-temperature (2T) hydrodynamics and molecular dynamics (MD). It is found that the rear-side spallation threshold F _s exceeds the front-side ablation threshold F _a. We propose to extend the common approach in laser-matter experiments by pump–probe measuring of the rear-side displacement.     

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.     

Femtosecond laser-induced damage of gold films

Single- and multi-shot ablation thresholds of gold films in the thickness range of 31-1400 nm were determined employing a Ti:sapphire laser delivering pulses of 28 fs duration, 793 nm center wavelength at 1 kHz repetition rate. The gold layers were deposited on BK7 glass by an electron beam evaporation process and characterized by atomic force microscopy and ellipsometry. A linear dependence of the ablation threshold fluence F_th on the layer thickness d was found for d ≤ 180 nm. If a film thickness of about 180 nm was reached, the damage threshold remained constant at its bulk value. For different numbers of pulses per spot (N-on-1), bulk damage thresholds of ∼0.7 J cm⁻² (1-on-1), 0.5 J cm⁻² (10-on-1), 0.4 J cm⁻² (100-on-1), 0.25 J cm⁻² (1000-on-1), and 0.2 J cm⁻² (10000-on-1) were obtained experimentally indicating an incubation behavior. A characteristic layer thickness of L_c ≈ 180 nm can be defined which is a measure for the heat penetration depth within the electron gas before electron-phonon relaxation occurs. L_c is by more than an order of magnitude larger than the optical absorption length of α⁻¹ ≈ 12 nm at 793 nm wavelength.     

Phonons in disordered solids

The effects of crystalline disorder on the frequency distribution and lifetimes of phonons are investigated. As the disorder parameter g characterizing the scattering of normal modes is increased to g>g_c, the normal mode spectrum becomes unstable against arbitrarily small nonlinearities while the ground state (if any) becomes increasingly degenerate. The bandwidth of the acoustic phonon spectrum increases with g, from a value ω_Dat g = 0 to 1.24ω_D at g_c. The speed of sound at long wavelengths decreases with increasing g; at threshold (g_c) it has decreased by some 29.3% from its value at g = 0. For g < g_c the scattering lifetime of long-wavelength normal modes satisfies Rayleigh's law (1/τ = A(_g)ω⁴). At g_c the damping satisfies a different law: 1/τ = Bω². Similar effects are obtained for the optic mode phonons. For these reasons, it appears that g_c marks the threshold of amorphous behavior, although the regime g >g_c is beyond the scope of our model.     

Enhancement of coercivity with reduced grain size in CoCrPt film grown by pulsed laser deposition

We report a pulsed laser deposition (PLD) growth of VMn/CoCrPt bilayer with a magnetic coercivity (H_c) of 2.2 kOe and a grain size of 12 nm. The effects of VMn underlayer on magnetic properties of CoCrPt layer were studied. The coercivity, H_c, and squareness, S, of VMn/CoCrPt bilayer, is dependent on the thickness of VMn. The grain size of the CoCrPt film can also be modified by laser parameters. High laser fluence used for CoCrPt deposition produces a smaller grain size. Enhanced H_c and reduced grain size in VMn/CoCrPt is explained by more pronounced surface phase segregation during deposition at high laser fluence.     

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.     

A single parameter scaling theory in a disordered layered system

We show that in a disordered layered system all states are localized if k_Fl<4Πg_c, irrespective of the interlayer coupling t _⊥. The crossover of dimensionality depends on t_⊥. Near the critical value t_⊥^c at which the Anderson transition occurs, the correlation length ζ^m and the localization length ζ^loc are calculated.     

Guidelines for efficient direct ablation of dielectrics with single femtosecond pulses

We provide guidelines to femtosecond laser users to select ad hoc laser parameters, namely the fluence and pulse duration, in the context of the development of ablation processes at the surface of dielectrics using single femtosecond pulses. Our results and discussion are based on a comprehensive experimental and theoretical analysis of the energy deposition process at the surface of fused silica samples and of their postmortem ablation characteristics, in the range of intensities from 10¹³ to 10¹⁵ W/cm². We show experimentally and numerically that self-induced plasma transient properties at the pulse timescale dramatically determine the efficiency of energy deposition and affect the resulting ablation morphology. In practice, we determine that the precise measurement of two characteristic fluence values, namely the laser-induced ablation threshold F _th,LIAT and the fluence F _opt for maximum ablation efficiency, are only required to qualify the outcomes of laser ablation at the surface of a dielectric in an extended range of applied fluence.     

Effect of the emitter temperature and emitter atom ionization potential on field evaporation

The field evaporation of nickel, nichrome alloy, and tungsten carbide at different temperatures is studied with a time-of-flight atomic probe and a field emission microscope. The charge of evaporating ions does not depend on the emitter temperature: it decreases with decreasing evaporating field F _ev. If F _ev does not vary with temperature, so does the charge of the ions. In the case of multicomponent emitters with different ionization potentials of the components, the components evaporate at the same values of F _ev in the form of atoms and ionized clusters. The reason for such behavior is that the initial evaporation of the easily ionizable component decreases the binding energy of harder-to-ionize ones to the point where they can evaporate at the same field.     

Swelling and modification of silicone surface by F2 laser irradiation

The surface of silicone rubber swelled and was modified by 157-nm F₂ laser irradiation at a laser fluence less than the ablation threshold. The irradiated surface swelled to a height of approximately 3 m. Fourier-transform infrared (FT-IR) spectroscopy and X-ray photoelectron spectroscopy showed that the irradiated surface was modified to SiO₂. 193-nm ArF laser irradiation of the silicone rubber induced the surface to swell, but not to modify to SiO₂. The IR peaks of end groups of silicone were observed in the FT-IR spectra of the surface. From these results, it is concluded that the main chains (Si-O) of silicone were photodissociated and generation of low molecular weight silicones caused the swelling. In addition, it was observed that methane and carbon dioxide were released from silicone rubber when each laser beam irradiated it. These gases were generated by photodissociation of the side chains (Si-CH₃) of silicone. An F₂ laser beam can photodissociate the Si-CH₃ bonds and the Si-O bonds of silicone and O₂ effectively even at a laser fluence less than the ablation threshold, resulting in the modification to SiO₂ and the swelling. PACS 61.80.Ba; 61.82.Pv; 82.50.Hp     

Searching for key parameter for determining Tc in Fe-based superconductors: Study of P/As substitution in RFe(P,As)(O,F) [R=La and Nd]

We have investigated the relation between the temperature-dependence of resistivity and superconducting transition temperature T_c in RFeP_1−xAs_xO_0.90F_0.10 (x=0-1.0) (R=La and Nd). In contrast to the linear change of the crystal structure with increasing x, the temperature dependence of resistivity and T_c show non-monotonous x-dependence. When the As concentration x is increased, the temperature-dependence of resistivity changes from T² to T-linear, and T_c distinctly increases in all the La compounds and the Nd ones with x<0.60. The results indicate that the substitution of As for P induces the spin fluctuation and resultantly enhances T_c. On the other hand, we could not find any relation between the temperature-dependence of resistivity and T_c in the Nd samples with x>0.60. This may suggest the existence of other parameters for determining T_c besides the antiferromagnetic correlation in this system.     

New results on the peierls transition of TTF-TCNQ by electron tunneling

We realized TTF-TCNQ(Al₂O₃)Al junctions with a point contact geometry using the TTF-TCNQ crystal as the point electrode. Junctions have been studied in the two different regimes, T>T_c and T<T_c. For T>T_c the numerically analyzed dynamic conductance shows a parabolic dependence which reflects the metallic regime. For T<T_c a clear deviation from the parabola has been pointed out and a rough estimation of the gap can be deduced from the “conductance well” width.     

Effect of electron-beam irradiation on the magnetic properties of Ga1−xMnxAs thin films grown on GaAs (100) substrates

The effect of electron-beam irradiation on the magnetic properties of (Ga_1−xMn_x)As thin films grown on GaAs (100) substrates by using molecular beam epitaxy was investigated. The ferromagnetic transition temperature (T_c) of the annealed (Ga_0.933Mn_0.067)As thin films was 160 K. The T_c value for the as-grown (Ga_0.933Mn_0.067)As thin films drastically decreased with increasing electron-beam current. This significant decrease in the T_c value due to electron-beam irradiation originated from the transformation of Mn substituted atoms, which contributed to the ferromagnetism, into Mn interstitials or Mn-related clusters. These results indicate that the magnetic properties of (Ga_1−xMn_x)As thin films grown on GaAs (100) substrates are significantly affected by electron-beam irradiation.