Identification of non-thermal and thermal processes in femtosecond laser-ablated aluminum

Non-thermal and thermal processes due to femtosecond laser ablation of aluminum (Al) at low, moderate, and high-fluence regimes are identified by Atomic Force Microscope (AFM) surface topography investigations. For this purpose, surface modifications of Al by employing 25 fs Ti: sapphire laser pulses at the central wavelength of 800 nm have been performed to explore different nano- and microscale features such as hillocks, bumps, pores, and craters. The mechanism for the formation of these diverse kinds of structures is discussed in the scenario of three ablation regimes. Ultrafast electronic and non-thermal processes are dominant in the lower fluence regime, whereas slow thermal processes are dominant at the higher fluence regime. Therefore, by starting from the ablation threshold three different fluence regimes have been chosen: a lower fluence regime (0.06–0.5 J cm^?2 single-shot irradiation under ultrahigh vacuum condition and 0.25–2.5 J cm^?2 single-shot irradiation in ambient condition), a moderate-fluence regime (0.25–1.5 J cm^?2 multiple-shot irradiation), and a high-fluence regime 2.5–3.5 J cm^?2 multiple-shot irradiation. For the lower fluence (gentle ablation) regime, around the ablation threshold, the unique appearance of individual, localized Nano hillocks typically a few nanometers in height and less than 100 nm in diameter are identified. These Nano hillock-like features can be regarded as a nonthermal, electronically induced phase transition process due to localized energy deposition as a result of Coulomb explosion or field ion emission by surface optical rectification. At a moderate-fluence regime, slightly higher than ablation threshold multiple-pulse irradiation produces bump-formation and is attributed to ultrafast melting (plasma formation). The high-fluence regime results in greater rates of material removal with highly disturbed and chaotic surface of Al with an appearance of larger protrusions at laser fluence well above the ablation threshold. These nonsymmetrical shapes due to inhomogeneous nucleation, cluster formation, and resolidification of a metallic surface after melting are attributable to slow thermal processes (ps time scale).     

Superresolved femtosecond laser ablation

The determinist behavior of the femtosecond ablation process allows morphing features well under the diffraction limit by utilizing the thresholding effect, down to the nanometer scale. Because there are a vast range of applications where scaling down the size of the features is a major concern, we investigate the use of superresolving pupil plane filters. As is well known, these filters redistribute the focused optical intensity for a narrower bright spot and, as a trade-off, increase the sidelobes. However, this drawback can be rendered insignificant if all the outer optical power is kept under the determinist threshold value. Two types of pure absorbing binary filter have been tried, giving credence to a size reduction of the ablations in fused silica.     

Model description of surface charging during ultra-fast pulsed laser ablation of materials

We present a model describing the dynamical mechanisms responsible for generating fast ion ejection under ultra-short pulsed laser irradiation. The model is based on a simplified drift–diffusion approach describing the evolution of the laser-generated charge carriers, their transport, and the electric field generated as a result of quasi-neutrality breaking in the irradiated target. The importance of different processes in generating the non-thermal material-ejection mechanisms is discussed. A common frame is applied to dielectrics, semiconductors, and metals and different dynamical behaviour is observed. The modelling results are in good agreement with fs pump–probe studies and measurements of the velocity distributions of the emitted ions.     

Table-top 50-W laser system for ultra-fast laser ablation

We have built a mode-locked Nd:YVO₄ laser with a very long resonator which produces an average power of 50 W in 13-ps pulses at 1064 nm and was designed for applications in micro-machining, the deposition of optical thin films, and the growth of nano-clusters in the laser-ablated plumes. By operating the laser at very low mode-locking repetition rates (1.5 MHz, 2.6 MHz, and 4.1 MHz), high pulse power is available in a near diffraction limited beam, allowing focused intensities to exceed 10¹² W/cm² and permitting efficient evaporation of difficult materials such as Si. The high power also allows conversion into the second harmonic at 532 nm with an efficiency exceeding 80%. Measurements of the ablation mass in experiments with metals show a 30–100 times increase in the ablation rate compared to the conventional low-repetition-rate ns-range lasers. PACS 79.20.Ds; 81.15.Fg; 81.16.Mk; 42.62.Cf     

单脉冲飞秒激光烧蚀炸药过程的热效应研究

飞秒激光能够在极短时间内烧蚀炸药产生高温高压等离子体。可以利用飞秒激光对含能材料或含能元器件进行精密加工。深入认识飞秒激光烧蚀炸药过程中,炸药内部的热效应是发展飞秒激光加工炸药技术的基础。建立了单脉冲飞秒激光烧蚀炸药过程的流固耦合计算模型,考虑了在高温高压等离子体和炸药自热反应的共同作用下,炸药内部的热效应。对飞秒激光烧蚀TNT炸药过程进行了流体力学数值模拟。计算结果表明：TNT炸药中未烧蚀区域产生了热效应,峰值温度高于TNT炸药的点火温度,但由于炸药内热效应区域极小,高温持续时间极短,因此炸药内温度迅速下降,没有发生点火现象。     

Lithographical laser ablation using femtosecond laser

Lithographical laser ablation was demonstrated using a femtosecond laser with a lithographical optical system. In this method, a femtosecond laser beam passes through a mask and the pattern is imaged on a film by a coherent optical system. As a result, the film is lithographically ablated, and a micron-sized pattern can be generated in a single shot. The resolution of generation was 13 m, and the narrowest width of a generated line was about 4 m. Moreover, the system was applied to transmission gratings as masks, and nano-sized periodic structures such as nano-sized hole matrices and nano-meshes were generated in a single shot. PACS 52.38.Mf; 42.25.Hz; 42.82.Cr; 81.16.-c     

Investigation of nanoparticle generation during femtosecond laser ablation of metals

The production of nanoparticles via femtosecond laser ablation of gold and copper is investigated experimentally involving measurements of the ablated mass, plasma diagnostics, and analysis of the nanoparticle size distribution. The targets were irradiated under vacuum with a spot of uniform energy distribution. Only a few laser pulses were applied to each irradiation site to make sure that the plume expansion dynamics were not altered by the depth of the laser-produced crater. Under these conditions, the size distribution of nanoparticles does not exhibit a maximum and the particle abundance monotonously decreases with size. Furthermore, the results indicate that two populations of nanoparticles exist within the plume: small clusters that are more abundant in the fast frontal plume component and larger particles that are located mostly at the back. It is shown that the ablation efficiency is strongly related to the presence of nanoparticles in the plume.     

Thermodynamic evolution of materials during laser ablation under pico and femtosecond pulses

Using molecular-dynamics, we study the thermodynamic evolution of a simple two-dimensional Lennard–Jones system during laser ablation for pulse durations ranging from 200 fs to 400 ps. We briefly review results previously obtained for fs pulses where the evolution of the material was shown to be solely a function of the locally absorbed energy (provided that only thermal effects are important), i.e., is adiabatic. For longer pulses (100 and 400 ps) the situation becomes more complex, as the relaxation path also depends on the position in the target and on the timescale on which expansion occurs. We show that, in contrast to fs pulses, the material ejected following ps laser irradiation does not enter the liquid–vapor metastable region before ablation occurs, hence showing that phase explosion is not the dominant mechanism in this regime. Following on from previous work, we propose that trivial fragmentation is the main ablation mechanism. PACS 79.20.Ds; 79.20.Ap; 61.80.Az     

Experimental investigation of ablation efficiency and plasma expansion during femtosecond and nanosecond laser ablation of silicon

Femtosecond laser (Ti:sapphire, 100 fs pulse duration) ablation of silicon in air was compared with nanosecond laser (Nd:YAG, 3 ns pulse duration) ablation at ultraviolet wavelength (266 nm). Laser ablation efficiency was studied by measuring crater depth as a function of pulse number. For the same number of laser pulses, the fs-ablated crater was about two times deeper than the ns-crater. The temperature and electron number density of the laser-induced plasma were determined from spectroscopic measurements. The electron number density and temperature of fs-induced plasmas decreased faster than ns-induced plasmas due to different energy deposition mechanisms. Images of the laser-induced plasma were obtained with femtosecond time-resolved laser shadowgraph imaging. Plasma expansion in both the perpendicular and the lateral directions were compared. PACS 52.38.Mf; 52.30.-q     

The influence of ultra-fast temporal energy regulation on the morphology of Si surfaces through femtosecond double pulse laser irradiation

The effect of ultra-short laser-induced morphological changes upon irradiation of silicon with double pulse sequences is investigated under conditions that lead to mass removal. The temporal delay between 12 double and equal-energy pulses (E _p=0.24 J/cm² each, with pulse duration t _p=430 fs, 800 nm laser wavelength) was varied between 0 and 14 ps and a decrease of the damaged area, crater depth size and periodicity of the induced subwavelength ripples (by 3–4 %) was observed with increasing pulse delay. The proposed underlying mechanism is based on the combination of carrier excitation and energy thermalization and capillary wave solidification and aims to provide an alternative explanation of the control of ripple periodicity by temporal pulse tailoring. This work demonstrates the potential of pulse shaping technology to improve ultra-fast laser-assisted micro/nanoprocessing.     

Nanoparticles size modifications during femtosecond laser ablation of nickel in vacuum

Nanoparticles were synthesized by irradiating a nickel target with femtosecond laser pulses in high vacuum, and subsequently analyzed. The proof-of-principle experiments aim to modify the size characteristics of the produced nanoparticles. For nickel it is found that: (i) ultraviolet laser pulses lead to a remarkable change in the nanoparticles size distribution with respect to visible laser pulses; (ii) irradiation of the femtosecond pulses induced ablation plume with a second, delayed ultraviolet laser pulse can change the size characteristics of the produced nanoparticles.     

Phase transitions in femtosecond laser ablation

In this study we simulate an interaction of femtosecond laser pulses (100 fs, 800 nm, 0.1-10 J/cm²) with metal targets of Al, Au, Cu, and Ni. For analysis of laser-induced phase transitions, melting and shock waves propagation as well as material decomposition we use an Eulerian hydrocode in conjunction with a thermodynamically complete two-temperature equation of state with stable and metastable phases. Isochoric heating, material evaporation from the free surface of the target and fast propagation of the melting and shock waves are observed. On rarefaction the liquid phase becomes metastable and its lifetime is estimated using the theory of homogeneous nucleation. Mechanical spallation of the target material at high strain rates is also possible as a result of void growth and confluence. In our simulation several ablation mechanisms are taken into account but the main issue of the material is found to originate from the metastable liquid state. It can be decomposed either into a liquid-gas mixture in the vicinity of the critical point, or into droplets at high strain rates and negative pressure. The simulation results are in agreement with available experimental findings.     

Dynamics of mid-infrared femtosecond laser resonant ablation

Resonant ablation is beneficial to avoiding uncontrollable subsurface damages in the laser ablation of polymers. In this paper the dynamics of mid-infrared laser resonant ablation of polylactic acid and toluene was calculated by using fluid dynamic equations. The merits and drawbacks of mid-infrared femtosecond laser resonant ablation of high molecular weight polymers have been discussed.     

Neutrals ejection in intense femtosecond laser ablation

Time-resolved shadowgraphs and holograms of intense femtosecond laser ablation of aluminum are reported. The different bending trends of interference fringes are found in the ablations of aluminum and other materials at probe wavelengths of 400 and 800 nm, for the first time to our knowledge, which could be attributed to the ejection of massive neutral droplets induced by critical-point phase separation during the second material ejection.     

Metal absorptivity in femtosecond pulsed laser ablation

In this paper, the effect of the absorptivity of metal on femtosecond pulsed laser ablation is investigated. The formulas for the absorptivity depending on target temperature are derived from Maxwell Equations and the Lambert-Beer’s law. Based on this, a new two-temperature model is proposed to describe the femtosecond pulsed laser ablation with metal. Then, using Au as an example, a finite difference method is employed to simulate the space-dependent and time-dependent absorptivity and the target temperature. The temperature evolution of our model is compared with the result obtained form the heat conduction model taking the absorptivity as constant. It is shown that the absorptivity plays an important role in the femtosecond pulsed laser ablation. The results of this paper are helpful in choosing the best technical parameters in femtosecond pulsed laser ablation.      

Probing particle synthesis during femtosecond laser ablation: initial phase transition kinetics

The impulsive superheating of matter by an intense, ultrashort laser pulse drives material expansion into vacuum (ablation) and an associated formation of nanoparticles. The underlying dynamics of particle formation are complex and direct experimental probes of the rapid material evolution are essential. Femtosecond lasers coupled to modern synchrotrons offer an important new opportunity to probe ejecta dynamics on an atomic lengthscale. Here, the impulsive heating of a semiconductor (silicon) by an intense femtosecond laser pulse leads to material ejection and time-resolved photoemission spectroscopy probes rapid solidification kinetics occurring within the ejecta. Transient photoemission peak-shifts indicate that material is ejected predominantly as liquid droplets and that solidification occurs rapidly (<50 ps). The solidification time suggests that vacuum ejection leads to significantly enhanced undercooling compared to what has been obtained by more conventional quenching techniques; this may be of interest in attempts to trap novel material states associated with extreme laser heating. Finally, a low fraction of vapor particles in the ejecta supports a view that the size-distribution of ejected particles is set by an initial fragmentation process rather than by vapor condensation. PACS 82.60.Qr; 87.64.Lg; 62.50.+p     

Nanosecond and femtosecond excimer laser ablation of fused silica

Ablation of fused silica using standard excimer lasers (20–30 ns pulse duration at 193, 248, and 308 nm) and a short pulse laser system (500 fs at 248 nm) is reported. Ablation rates range from several hundred nm/pulse (193 nm or fs-laser) up to about 6 m/pulse (308 nm). The performance of the ablation is found to depend not only on wavelength and pulse duration but also on the existing or laser induced surface quality (e.g., roughness) of the material. Special ablation phenomena are observed. At 193 nm and moderate fluence (3 J/cm²) ablation takes place at the rear side of a plate without affecting the front side, whereas at higher fluence normal ablation at the front side occurs. At 248 nm (standard excimer) the existence of two consecutive ablation phases is observed: smooth ablation at low rate is followed by explosive ablation at high rate. Using fs-pulses smooth shaped holes are formed during the first pulses, whereas high pulse numbers cause the development of a ripple structure in the ablation craters.The results lead to the conclusion that two different ablation mechanisms are involved: the first is based on two photon bulk absorption, the second on controlled surface damage in relation with (partially laser induced) singularity conditions at the surface.Presented at LASERION '91, June 12–14, 1991, München (Germany)