Early stage of the material removal during ArF laser ablation of graphite

Material removal during ArF excimer laser ablation of graphite at atmospheric pressure was investigated by two independent methods; 1) by observation of the propagating properties of the shock wave generated by the carbonaceous ejecta and 2) by in situ measurement of the size distribution of carbon nanoparticles condensing in the ablation plume. This latter was carried out by a scanning mobility particle sizer system based on a differential mobility analyser. The performed measurements indicate that the material removal during ArF laser ablation consists of two steps at fluences above the threshold fluence. First, a thin layer of carbon (of the order of 1 nm) is removed by a quick desorption process, leading to shockwave formation. This process takes place in a ns time scale, and desorption rate estimations reveal that this can not be explained by thermal surface evaporation. Since to our knowledge there is no thermal process that could account for the estimated desorption rate, it is argued that this is a fast photochemical (i.e. non-thermal) process. The size distribution of the condensed nanoparticles related to this step shows a rising edge at diameters below 10 nm. At fluences above the ablation threshold, the majority of the material is ejected in the second phase, resulting in condensation of carbon nanoparticles, peaking at 50 nm diameters in the size spectrum. Both shockwave formation and material removal are also detected well below the ablation threshold fluence, which is attributed to the photochemical process. PACS 61.46.+w; 81.16.Mk     

Laser backside etching of fused silica due to carbon layer ablation

The backside ablation of a absorbing carbon layer onto fused silica is studied in air and water confinement in comparison. The confinement influences the etch rate and the laser fluence dependence of the etch rate significantly while the threshold fluence is almost the same. The different confinement of the laser induced plasma results in the observed rate saturation in the case of air and in a linear growing rate in the case of water confinement at medium laser fluences. The less dense air confinement permits a faster plasma expansion of the laser plume than in the case of water confinement and effects consequently the interaction time and interaction strength of the laser plume with the fused silica surface. The differences in the laser-plasma-substrate interaction cause the observed rate saturation at weak interaction (air) and the growing etch rate at strong interaction (water). Thus, the confinement situation controls the interaction process in the case of backside ablation and should be considered in indirect material processing methods such as LIBWE and LESAL, too. PACS 81.65.C; 81.05.K; 79.20.D; 61.80.B; 42.55.L; 68.45.D     

Features of plasma plume evolution and material removal efficiency during femtosecond laser ablation of nickel in high vacuum

We present an experimental characterization describing the characteristics features of the plasma plume dynamics and material removal efficiency during ultrashort, visible (527 nm, ≈300 fs) laser ablation of nickel in high vacuum. The spatio-temporal structure and expansion dynamics of the laser ablation plasma plume are investigated by using both time-gated fast imaging and optical emission spectroscopy. The spatio-temporal evolution of the ablation plume exhibits a layered structure which changes with the laser pulse fluence F. At low laser fluences (F<0.5 J/cm²) the plume consists of two main populations: fast Ni atoms and slower Ni nanoparticles, with average velocities of ≈10⁴ m/s for the atomic state and ≈10² m/s for the condensed state. At larger fluences (F>0.5 J/cm²), a third component of much faster atoms is observed to precede the main atomic plume component. These atoms can be ascribed to the recombination of faster ions with electrons in the early stages of the plume evolution. A particularly interesting feature of our analysis is that the study of the ablation efficiency as a function of the laser fluence indicates the existence of an optimal fluence range (a maximum) for nanoparticles generation, and an increase of atomization at larger fluences. PACS 52.50.-b; 52.38.Mf; 79.20.Ds; 81.07.-b     

超短脉冲激光烧蚀石墨产生的喷射物的时间分辨发射光谱研究

本文使用不同激光能流(18 J/cm²–115 J/cm²)和脉冲宽度(50 fs–4 ps)的超短脉冲激光在真空中(4×10^-4 Pa)烧蚀高定向热解石墨. 通过测量烧蚀喷射物的时间分辨发射光谱研究喷射物的超快时间演化. 在喷射物发射光谱中, 观察到了C₂基团的天鹅带光谱系统, 416 nm附近C₁₅基团的由电子能级¹Σ_u⁺ 和¹Σ_g⁺之间的振动跃迁产生的光谱峰以及连续谱. 50 fs, 115 J/cm²的脉冲激光烧蚀产生的喷射物的连续谱的强度衰减分为快速下降和慢速下降两个阶段(以20 ns时间延迟为分界). 这表明连续谱是由两种不同的组分贡献的. 快速下降阶段, 连续谱主要由碳等离子体通过韧致辐射产生; 慢速下降阶段, 连续谱主要由烧蚀后期产生的大颗粒碳簇的热辐射贡献. 实验结果还揭示了激光能流的提高, 会明显增加喷射物中碳等离子体和激发态C₂的含量, 但对质量稍大的C₁₅的影响较小; 此外, 50 fs脉冲激光烧蚀产生的连续谱的存在时间会随着激光能流的减小而增大, 这说明低能流更有利于在烧蚀后期产生碳簇. 脉宽主要影响喷射物连续谱的时间演化. 4 ps脉冲激光烧蚀产生的连续谱的整个时间演化过程明显慢于50 fs脉冲产生的连续谱.     

Silicon cluster formation in the laser ablation of SiO at 308 nm

Neutral silicon cluster formation in the laser (308 nm) ablation of silicon monoxide was investigated through the analysis of composition and dynamics of the ablation plume under different laser fluence conditions. The neutral species were ionized by a second laser (193 nm) and the positionized species detected by TOF-MS (time-of-flight mass spectrometry). At low laser fluences, plume composition is dominated by SiO; above 0.6 J/cm² Si, SiO and Si₂ have comparable intensity and Si_n (n≤7) clusters are observed. Flow velocities and temperatures of the ejected species are nearly mass-independent, indicating that the plume dynamics are close to the strong expansion limit, implying a collisional regime. Through the relation between the estimated values of terminal flow velocity and surface temperature, u_T²∝T_S, it is found that, at low laser fluences, the surface temperature increases linearly with laser fluence, whereas, at the laser fluence at which Si_n clusters are observed, the increase of temperature is below the linear dependence. The population distribution of the ejected Si_n provides some indication of a formation mechanism based on condensation. Analogies between the ablation behavior of silicon monoxide and silicon targets are considered. PACS 82.30.Nr; 81.05.Gc; 78.70.-g     

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.     

Evolution of the deposition rate during pulsed laser deposition of hydroxyapatite coatings and its relation with target morphology

The evolution of the deposition rate during pulsed laser deposition of hydroxyapatite coatings with a KrF excimer laser was studied. This evolution was related to the changes produced on the target morphology during laser irradiation. Laser fluences in the 1.0–5.2 J/cm² range, typical for the deposition of hydroxyapatite coatings, were investigated. Deposition rates were measured through a quartz-crystal microbalance, and the target surface was observed by scanning electron microscopy. At the lowest fluences, the deposition rate decreases as the number of pulses increases. At the same time, a cone structure is developed on the target surface. At the highest fluences, the deposition rate increases with the number of pulses. In this case, the target surface becomes rough but cones are not formed. In all cases, an enlargement of the effective irradiated area results. This enlargement produces the effect of fluence dilution and also an increase of the emitting area. These opposite effects could account for the different evolutions found for the deposition rate. At low fluences the effect of fluence dilution would predominate over the increase of the emitting area, and at high fluences the second effect would predominate over the first. Received: 28 September 2000 / Accepted: 4 October 2000 / Published online: 10 January 2001     

Double-pulse femtosecond laser ablation of the surface of stainless steel with variable interpulse delays

Spectral studies of optical emission from plumes produced via ablation of the surface of stainless steel in the phase explosion regime at different incident fluences by a pair of collinear degenerate femtosecond laser pulses, separated by variable delay time of 0.01–1.5 ns, demonstrate a drastic decrease in atomic emission intensities in a subnanosecond range. This effect was related to “bulk” absorption of the second pump pulse in ablative plumes with near-critical density, achieved during their hydrodynamic expansion on a subnanosecond timescale.     

Angular distributions of plume components in ultrafast laser ablation of metal targets

In view of its fundamental interest and relevance to nanoparticle film production, we have characterised the nanoparticle component of the ablation plume generated in femtosecond laser irradiation of metals. The results are compared to those of the ion plume, which is considered as representative of the atomic component. At moderate laser fluences, the angular distributions of both nanoparticle and ionic components were studied by measuring the spatial distribution of deposition on a transparent substrate and with a planar Langmuir probe, respectively. Our results show that both angular profiles of the plume components can be described by Anisimov model of isentropic expansion. As the laser fluence is increased above a value of several times the ablation threshold, the shape of the nanoparticle angular distribution progressively differs from the Anisimov prediction, contrary to what is observed for the ion component. This effect is interpreted in terms of the influence of the pressure exerted by the nascent atomic plasma plume on the initial hydrodynamic evolution of nanoparticle material.     

Dynamics of the ejected material in ultra-short laser ablation of metals

A molecular dynamics model is applied to study the formation and the early stages of ejection of material in ultra-short laser ablation of metals in vacuum. Simulations of the ablation process for iron at a pulse duration of 0.1 ps and at different laser fluences are performed. Different features of the ejection mechanism are observed below, near, and above the ablation threshold. The last is estimated as approximately 0.1 J/cm². The structure of the ablated material is found to depend on the applied laser fluence. The expanded plume consists mainly of large clusters at fluences near to the threshold. With the increase of the laser fluence the presence of the large clusters decreases. Clear spatial segregation of species with different sizes is observed in the direction normal to the surface several tens of picoseconds after the laser pulse onset. The angular distribution of the ejected material is estimated for different regimes of material removal. Above the ablation threshold the distribution is forward peaking. PACS 79.20.Ds; 52.38.Mf; 02.70.Ns; 81.05.Bx     

Hydrodynamic instability and self-organization of a submicron relief on metal surfaces upon femtosecond laser exposure in liquids

Multishot exposure of nickel and iron surfaces by loosely focused femtosecond laser pulses in isopropyl alcohol resulted in quasi-regular arrays of submicron spikes and other intermediate self-organized structures. Such self-organized surface relief is considered to be formed via hydrodynamic instability of molten metallic surfaces in their contact with a near-critical alcohol vapor layer with the pressure of about 5 MPa.     

Impact of open de-ionized water thin film laminar immersion on the liquid-immersed ablation threshold and ablation rate of features machined by KrF excimer laser ablation of bisphenol A polycarbonate

Debris control and surface quality are potential major benefits of sample liquid immersion when laser micromachining; however, the use of an immersion technique potentially modifies the ablation mechanism when compared to an ambient air interaction. To investigate the machining characteristics, bisphenol A polycarbonate has been laser machined in air and under a controllable open liquid film. To provide quantitative analysis, ablation threshold, ablation rate and the attenuation coefficient of the immersing de-ionized (DI) water fluid were measured. In ambient air the threshold fluence was measured to be 37 mJ cm⁻². Thin film immersion displayed two trends: threshold fluences of 58.6 and 83.9 mJ cm⁻². The attenuation of DI water was found to be negligible; thus, the change in ablation rate resulted from increased confinement of the vapour plume by the liquid medium, generating higher Bremsstrahlung attenuation of the beam, lowering the laser etch rate. Simultaneously, splashing motivated by the confined ablation plume allowed release of plume pressure before plume etching commenced. This contributed to the loss of total etching efficiency. Two interaction scenarios were obsereved as a result of splashing: (i) intermediate threshold fluence, where splashing occured after every pulse in a mode that interrupted the flow entirely, leaving an ambient air interaction for the following pulse; (ii) high threshold fluence, where splashing occured for every pulse in a mode that allowed the flow to recommence over the image before the next pulse causing every pulse to experience Bremsstrahlung attenuation. Since attenuation of the immersion liquid was negligible, it is the action of the constrained ablation plume within a thin flowing immersion liquid, the resultant Bremsstrahlung attenuation and splashing events that are the critical mechanisms that modify the primary ablation characteristics.     

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.     

Pulsed laser-induced ablation of absorbing liquids and acoustic-transient generation

2 CrO₄ are irradiated by a KrF excimer laser (λ=248 nm, FWHM=24 ns) with moderate energy density (up to 100 MW/cm²) below the plasma-formation threshold. The ablation process, including the vapor-cavity formation and the acoustic-wave propagation is visualized by laser-flash photography. The ablation thresholds are determined by measuring the generated pressure transients and vapor-phase kinetics using a broadband piezoelectric pressure transducer and a simultaneous optical-transmission probe, respectively. The mechanisms of liquid ablation and acoustic-pulse generation are investigated based on the thermoelastic behavior of the liquid medium and the evaporation dynamics. A numerical model is proposed to describe the explosive-vaporization process at high laser fluences. The computation results are compared with the experiment. In short-pulse heating, ablation can be initiated at low laser fluences by the tensile component of the thermoelastic stress without a significant increase in the liquid temperature. On the other hand, if the heating rate is rapid enough to achieve a high degree of superheating of the liquid, the abrupt increase of the homogeneous-bubble-nucleation rate leads to explosive vaporization, which then plays the major role in the ablation dynamics. The pressure transient in the liquid is generated thermoelastically at low laser fluences, but the contribution of the vapor-phase expansion and/or the recoil momentum exerted by the ablation plume becomes significant at high laser fluences. Shock waves are formed in the ambient air in the case of explosive vaporization. The propagation of these wave fronts is in good agreement with the numerical-computation results. Received: 8 February 1998/Accepted: 10 February 1998     

Laser surface treatment of screen-printed carbon nanotube emitters for enhanced field emission

This paper investigates the surface treatment of screen-printed carbon nanotube (CNT) emitters using a 248 nm (KrF) excimer laser. The field emission characteristics of the CNT emitters are measured following irradiation using laser fluences ranging from 80 to 400 mJ/cm². The results show that the turn-on electric field, the current density, and the distribution of the emission sites are highly dependent on the value of the laser fluence and are optimized at a fluence of 150 mJ/cm². Two distinct laser fluence regimes are identified. In the low fluence regime, i.e. 80-150 mJ/cm², the surface treatment process is dominated by a photo ablation mechanism, which results in the gradual removal of the binding material from the cathode surface and leads to an improvement in the emission characteristics of the CNT cathodes with an increasing fluence. However, in the high fluence regime, i.e. 150-400 mJ/cm², the thermal ablation mechanism dominates; resulting in a removal of the CNTs from the cathode surface and a subsequent degradation in the emission characteristics.     

Phenomenology of picosecond heating and evaporation of silicon surfaces coated with SiO2 layers

Picosecond time-resolved reflectivity measurements on bare silicon surfaces and silicon surfaces with oxide layers reveal very fast heat diffusion and material evaporation on subnanosecond time scales. With a thick oxide layer resolidification of a molten silicon surface can take place in a few hundred picoseconds. At high laser fluences, vaporization processes take only a couple of 100 ps.     

Laser opto-acoustic study of phase transitions in metals confined by transparent dielectric

First-order phase transitions in metal induced by nanosecond laser pulse are studied here. The metal surface is irradiated through a layer of transparent dielectric??an optical glass. Such confinement considerably increases the efficiency of pressure generation at the metal surface. This technique allows to obtain near-critical states of metals??with temperatures ??10⁴ K and pressures ??10⁴ atm with table-top equipment. At the same time the glass prevents the ablation plume formation??so the surface temperature can be measured using thermal radiation data. An experimental setup for simultaneous measurements of pressure, temperature and reflectivity was assembled based on the elaborated method of experimental research. The processes of melting of lead and boiling of mercury were studied. The onset of the phase transition process led to a considerable tightening of the pressure pulse. A substantial drop of surface reflectivity due to increase of temperature and decrease of density was observed.     

Laser ablation of liquid surface in air induced by laser irradiation through liquid medium

The pulse laser ablation of a liquid surface in air when induced by laser irradiation through a liquid medium has been experimentally investigated. A supersonic liquid jet is observed at the liquid–air interface. The liquid surface layer is driven by a plasma plume that is produced by laser ablation at the layer, resulting in a liquid jet. This phenomenon occurs only when an Nd:YAG laser pulse (wavelength: 1064 nm) is focused from the liquid onto air at a low fluence of 20 J/cm². In this case, as Fresnel’s law shows, the incident and reflected electric fields near the liquid surface layer are superposed constructively. In contrast, when the incident laser is focused from air onto the liquid, a liquid jet is produced only at an extremely high fluence, several times larger than that in the former case. The similarities and differences in the liquid jets and atomization processes are studied for several liquid samples, including water, ethanol, and vacuum oil. The laser ablation of the liquid surface is found to depend on the incident laser energy and laser fluence. A pulse laser light source and high-resolution film are required to observe the detailed structure of a liquid jet.