Identification of ultra-fast electronic and thermal processes during femtosecond laser ablation of Si

Ultra-fast electronic and thermal processes for the energy deposition mechanism during femtosecond laser ablation of Si have been identified by means of atomic force microscopy and Raman scattering techniques. For this purpose, Si targets were exposed with 800-nm, 25-fs Ti:sapphire laser pulses for different laser fluencies in air and under UHV (ultra high vacuum) conditions. Various nano- and microstructures on the surface of the irradiated samples are revealed by a detailed surface topography analysis. Ultra-fast electronic processes are dominant in the lower-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 UHV 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 higher-fluence regime (2.5–3.5 J?cm^?2 multiple-shot irradiation). Around the ablation threshold fluence, most significant features identified at the Si surface are nanohillock-like structures. The appearance of these nanohillocks is regarded as typical features for fast electronic processes (correlated with existence of hot electrons) and is explained on the basis of Coulomb explosion. The growth of these typical features (nanohillocks) by femtosecond laser irradiation is an element of novelty. At moderate irradiation fluence, a ring-shaped ablation with larger bumps and periodic surface structures is observed and is considered as a footprint of ultra-fast melting. Further increase in the laser fluence, i.e. a higher-fluence regime, resulted in strong enhancement of the thermal process with the appearance of larger islands. The change in surface topography provides an innovative clue to differentiate between ultra-fast electronic processes, i.e. Coulomb explosion (sub-100 fs) at a lower-fluence regime and ultra-fast melting (hundreds of fs) at a moderate-fluence regime, and slow thermal processes (ps time scale) at a higher-fluence regime. These fast electronic and thermal processes are well correlated to structural and crystallographic alterations, inferred from Raman spectroscopy.     

Laser induced mixing in multilayered Ti/Ta thin film structures

The possibility of interlayer mixing in a Ti/Ta multilayer system, induced by laser irradiation, was the main purpose of these experiments. Ti/Ta multilayer system, consisting of ten alternating Ti and Ta thin films and covered by slightly thicker Ti layer, was deposited on Si (100) wafers to a total thickness of 205 nm. Laser irradiation was performed in air by picoseconds Nd:YAG laser pulses in defocused regime with fluences of 0.057 and 0.11 J cm^?2. Laser beam was scanned over the 5?×?5 mm surface area with different steps along y-axes. Structural and compositional characterisation was done by auger electron spectroscopy, X-ray photoelectron spectroscopy, atomic force microscopy, and scanning electron microscopy. Laser processing at lower fluence caused only oxidation of the top Ti layer, despite of the number of applied laser pulses. Interlayer mixing was not observed. Application of laser pulses at fluence of 0.11 J cm^?2 caused partial and/or complete ablation of deposited layers. In partially ablated regions considerable mixing between Ti and Ta films was registered.     

Dependence of ablation threshold and LIPSS formation on copper thin films by accumulative UV picosecond laser shots

The ablation threshold and Laser-induced periodic surface structure (LIPSS) formation on copper thin film were investigated using a picosecond laser (Nd:YAG laser: 266 nm, 42 ps, 10 Hz). We show that the ablation threshold varies with respect to the number of laser shots (N) on two different substrates. The single-shot ablation threshold was estimated to be close to 170 ± 20 mJ/cm². The incubation coefficient was estimated to be 0.68 ± 0.03 for copper thin films on silicon and glass substrates. In addition, morphology changes of the ablated regions, in the same spot area, were studied as a function of fluence and number of laser shots. An intermediate structure occurred with a mix of low spatial frequency LIPSS (LSFL), high spatial frequency LIPSS (HSFL) and regular spikes at a fluence F < 250 mJ/cm² and 1,000 < N ≤ 10.000 shots. LSFL was observed with a spatial period close to the irradiation wavelength and an orientation perpendicular to the laser polarization, and HSFL with a spatial period of ～120 nm and a parallel orientation. Lastly, the global relationship between the laser parameters (i.e. fluence and number of shots) and LIPSS formation was established in the form of a 2D map.     

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.     

Surface topography of ultrashort laser-irradiated CaF2

A single-crystal CaF₂ (111) was irradiated with single and multiple laser (Ti:sapphire, 800 nm, 25 fs) shots at fluences ranging from 0.25 to 1.5 J cm^?2. In this fluence regime, a single laser pulse usually leads to typical bump-like features ranging from 200 nm to 1.5 μm in diameter and 10–50 nm in height. These bumps are related to compressive stresses due to a pressure build-up induced by fast laser heating and their subsequent relaxation. When CaF₂ is irradiated with successive (in our case 20) shots at a laser fluence of 1.5 J cm^?2, nanocavities at the top of the microbumps are observed. The formation of these nanocavities is regarded as an explosion and is attributed to the explosive expansion generated by shock waves due to laser-induced plasma after the nonlinear absorption of the laser energy by the material. Such kinds of surface structures at the nanometre scale could be attractive for nanolithography.     

Studies of some physical properties of PrFe0.7Ni0.3O3 thin films after 200 MeV Ag15+ irradiation

PrFe_0.7Ni_0.3O₃ thin films (thickness ~ 200 nm) were prepared by pulsed laser ablation technique on LaAlO₃ substrate. These films were irradiated with 200?MeV Ag¹⁵⁺ ions at various fluencies, ranging from 1 × 10¹¹ to 1 × 10¹² ions/cm². These irradiated thin films were characterized by using X-ray diffraction, dc conductivity, dc magnetization and atomic force microscopy. These films exhibit orthorhombic structure and retain it even after irradiations. The crystallite size (110–137?nm), micro strain (1.48 × 10^?2–1.75 × 10^?2 line^?2?m^?4) and dislocation density (79.7 × 10¹⁴–53.2 × 10¹⁴ line/m²) vary with ion fluencies. An enhancement in resistivity at certain fluence and then a decrease in its value (0.22175–0.21813?Ω?cm) are seen. A drastic change in observed magnetism after ion irradiation is seen. With ion irradiation, an increase in surface roughness, due to the formation of hillocks and other factors, is observed. Destruction of magnetic domains after irradiation can also be visualized with magnetic force microscopy and is in close agreement with magnetization data. The impact on various physical properties in these thin films after irradiation indicates a distortion in the lattice structure and consequently on single-particle band width caused by stress-induced defects.     

Swift heavy ion provoked structural, optical and electrical properties in SnO2 thin films

SnO₂ thin films grown on glass substrates at 300 ^°C by reactive thermal evaporation and annealed at 600 ^°C were irradiated by 120 MeV Ag⁹⁺ ions. Though irradiation is known to induce lattice disorder and suppression of crystallinity, we observe grain growth at a certain fluence of irradiation. X-ray diffraction (XRD) revealed the crystalline nature of the films. The particle size estimated by Scherrer’s formula for the irradiated films was in the range 10–25 nm. The crystallite size increases with increase in fluence up to 1×10¹² ions?cm^?2, whereas after that the size starts decreasing. Atomic force microscope (AFM) results showed the surface modification of nanostructures for films irradiated with fluences of 1×10¹¹ ions?cm^?2 to 1×10¹³ ions?cm^?2. The UV–visible spectrum showed the band gap of the irradiated films in the range of 3.56 eV–3.95 eV. The resistivity decreases with fluence up to 5×10¹² ions?cm^?2 and starts increasing after that. Rutherford Backscattering (RBS) reveals the composition of the films and sputtering of ions due to irradiation at higher fluence.     

Single and multiple shot near-infrared femtosecond laser pulse ablation thresholds of copper

The single-shot ablation threshold and incubation coefficient of copper were investigated using an amplified near-infrared, femtosecond Ti:sapphire laser. To date, the near-infrared femtosecond ablation threshold of copper has been reported in the range of several hundred millijoules per cm² based primarily on multiple shot ablation studies. A careful study of the single shot ablation threshold for copper was carried out yielding an incident single-shot ablation threshold of (1.06±0.12) J/cm² for a clean copper foil surface. This was determined by measuring the diameters of the ablation spots as a function of the laser pulse energy using scanning electron microscopy for spatially Gaussian laser spots. When multiple shots were taken on the same spot, a reduction in ablation threshold was observed, consistent with a multiple shot incubation coefficient of 0.76±0.02. Similar experiments on 250 nm and 500 nm copper thin films sputtered on a silicon substrate demonstrated that scaling the threshold values with the absorbance of energy at the surface yields a consistent absorbed fluence threshold for copper of (59±10) mJ/cm². This absorbed threshold value is consistent with the expected value from a two-temperature model for the heating of copper with an electron-lattice coupling constant of g=10¹⁷ Wm^-3 K^-1. Single-shot rippling of the surface in the threshold ablation intensity regime was also observed for the foil target but not for the smooth thin film target. PACS 61.80.Ba; 61.82.Bg     

Surface modulation of silicon surface by excimer laser at laser fluence below ablation threshold

Controlled single step fabrication of silicon conical surface modulations on [311] silicon surface is reported utilizing KrF excimer laser [λ=248 nm] at laser fluence below ablation threshold laser fluence. When laser fluence was increased gradually from 0 to 0.2 J/cm² for fixed 200 numbers of shots; first nanopores are observed to form at 0.1 J/cm², then very shallow nanocones evolve as a function of laser fluence. At 0.2 J/cm², nanoparticles are observed to form. Up to 0.15 J/cm² the very shallow nanocone volume is smaller but increases at a fast rate with laser fluence thereafter. It is observed that the net material volume before and after the laser irradiation remains the same, a sign of the melting and resolidification without any ablation.     

Formation of periodic structures by surface treatments of polyamide fiber: Part I. UV excimer laser irradiation

The processes of UV excimer laser irradiation (both high- and low-fluence) of polyamide fiber were systemically studied, including the surface temperature of the material during the treatment and possible mechanisms for the structure formation. The fluence applied in the high-fluence laser irradiation was above the ablation threshold of the material. The ablation of polymer can be described on the basis of photo-thermal bond breaking within the bulk material. The fluence applied in the low-fluence laser irradiation was far below the ablation threshold of the material. The development of low-fluence laser-induced structures is closely related to the absorption coefficient of the material, the laser fluence used, the polarization of the laser beam, the angle of incidence, and the number of laser pulses applied.     

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.     

Circular ripple formation on the silicon wafer surface after interaction with linearly polarized femtosecond laser pulses in air and water environments

Ultrashort laser pulse interaction with the surface of silicon wafer in air and water environments is investigated. Ti:sapphire laser with 40 femtosecond laser pulses at 790 nm and 10 Hz repetition rate was used. The ablation threshold of the silicon surface in the air was determined to be about 0.28 J cm^?2. The surface morphology was studied by using scanning electron microscope images. The size of the regular ripples formed in the air environment is a little smaller than the laser wavelength. Due to the nonlinear interaction and self-focusing before the target, the ripples size reduced to nearly a half of the laser wavelength in the water. Moreover, the spikes’ structure formation and their diameter in air and water were studied. Two regimes for spike formation in water are proposed that can explain the anomalous decrease of the spikes’ diameter in higher fluence. During the interaction of single linearly polarized femtosecond laser pulse with the surface, an irregular ripple formation that called circular ripple is observed. This structure which is a result of radiation pressure implies to the surface by the end of the pulse. A new physical model for interpretation of the circular ripples formation based on the ponderomotive force of an ultrashort pulse laser is proposed which can predict the size of the circular ripples. The calculated results are in accordance with our experimental findings.     

Drilling rate of five metals with picosecond laser pulses at 355, 532, and 1064 nm

Experimental results on picosecond laser processing of aluminum, nickel, stainless steel, molybdenum, and tungsten are described. Hole drilling is employed for comparative analysis of processing rates in an air environment. Drilling rates are measured over a wide range of laser fluences (0.05–20?J/cm²). Experiments with picosecond pulses at 355?nm are carried out for all five metals and in addition at 532?nm, and 1064?nm for nickel. A comparison of drilling rate with 6-ps and 6-ns pulses at 355?nm is performed. The dependence of drilling rate on laser fluence measured with picosecond pulses demonstrates two logarithmic regimes for all five metals. To determine the transition from one regime to another, a critical fluence is measured and correlated with the thermal properties of the metals. The logarithmic regime at high-fluence range with UV picosecond pulses is reported for the first time. The energy efficiency of material removal for the different regimes is evaluated. The results demonstrate that UV picosecond pulses can provide comparable quality and higher processing rate compared with literature data on ablation with near-IR femtosecond lasers. A significant contribution of two-photon absorption to the ablation process is suggested to explain high processing rate with powerful UV picosecond pulses.     

Enhancement in electrochemical properties of ionic liquid-based nanocomposite polymer electrolytes by 100 MeV Si9+ swift heavy ion irradiation

Swift heavy ion (SHI) irradiation has been used as a tool to enhance the electrochemical properties of ionic liquid-based nanocomposite polymer electrolytes dispersed with dedoped polyaniline (PAni) nanorods; 100 MeV Si⁹⁺ ions with four different fluences of 5?×?10¹⁰, 1?×?10¹¹, 5?×?10¹¹, and 1?×?10¹² ions cm^?2 have been used as SHI. XRD results depict that with increasing ion fluence, crystallinity decreases due to chain scission up to fluence of 5?×?10¹¹ ions cm^?2, and at higher fluence, crystallinity increases due to cross-linking of polymer chains. Ionic conductivity, electrochemical stability, and dielectric properties are enhanced with increasing ion fluence attaining maximum value at the fluence of 5?×?10¹¹ ions cm^?2 and subsequently decrease. Optimum ionic conductivity of 1.5?×?10^?2 S cm^?1 and electrochemical stability up to 6.3 V have been obtained at the fluence of 5?×?10¹¹ ions cm^?2. Ac conductivity studies show that ion conduction takes place through hopping of ions from one coordination site to the other. On SHI irradiation, amorphicity of the polymer matrix increases resulting in increased segmental motion which facilitates ion hopping leading to an increase in ionic conductivity. Thermogravimetric analysis (TGA) measurements show that SHI-irradiated nanocomposite polymer electrolytes are thermally stable up to 240–260 °C.     

Ultra-short pulse laser ablation of metals: threshold fluence, incubation coefficient and ablation rates

In this paper we present femtosecond laser ablation studies of the metals copper, silver and tungsten. Measurements of the threshold fluence determined from the hole diameters versus fluence provide incubation coefficients of the three materials, which are found to be equal within one standard deviation. Furthermore, we have determined the single-shot threshold fluences to be 1.7±0.3 J/cm², 1.5±0.4 J/cm² and 0.44±0.02 J/cm² for copper, silver and tungsten, respectively. These are in good agreement with theoretical values calculated neglecting heat diffusion.     

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.     

Surface modification and adhesion of wood-plastic composite (WPC) treated with UV/ozone

Because of the surfaces of wood-plastic composite (WPC) materials are enriched in polymers of low surface energy, they exhibit low adhesion properties. UV/ozone is proposed as surface treatment for increasing the surface energy and adhesion of WPC materials made with different polymers (polyethylene, polypropylene and polyvinyl chloride). UV lamp-WPC surface distance and time of UV exposure were varied for optimizing UV/ozone treatment of WPC, and UV dose used ranged between 2.02 × 10^?14 and 5.05 × 10^?12 J·s/m². UV/ozone treatment created new carbon-oxygen polar groups in WPC surfaces and increased their surface energy, mainly their polar component. Furthermore, ablation of the outermost WPC surface was produced, more noticeably by reducing the distance between WPC surface and UV lamp and by increasing the duration of the treatment. Noticeable increase in 180° peel adhesion was obtained in the joints made with UV/ozone treated WPC at 10–30 mm distance during 1–5 min (i.e., UV dose between 5.61 × 10^?14 and 2.53 × 10^?12 J·s/m²). Although 180° peel strength of joints made with acrylic adhesive tape and UV/ozone treated WPC for 10 min and 10 mm distance (UV dose: 5.05 × 10^?12 J·s/m²) was not increased because of dominant effect of ablation over creation of polar groups, the cross-hatch adhesion to different coatings was highly improved, irrespective of the polymer used and the wood content of WPC; however, the surface modifications and adhesion of UV/ozone treated WPC were more marked when its wood content was higher and by using UV dose between 0.10 × 10^?12 and 2.53 × 10^?12 J·s/m².     

Laser pulses designed in time by adaptive hydrodynamic modeling for optimizing ultra-fast laser–metal interactions

Determining optimal temporal pulse shapes is an essential aspect for controlling the nature and the energetic characteristics of the ablation products following laser irradiation of materials on ultra-fast scales. In this respect, adaptive feedback loops based on temporal pulse manipulation have been inserted into a hydrodynamic code. The procedure enables us to reach the theoretical maximal temperature at a certain energy input. Several regimes have been considered with fluences ranging from the ablation threshold (F _th=0.34 J/cm²) up to 10 J/cm², proposing an optimal coupling for laser–solid and laser–plasma interactions in these fluence regimes. We determine shapes of optimal pulses on ultra-short and short scales (up to 42 ps) and forecast optimized interaction scenarios with fundamental control factors difficult to access experimentally. Simulations performed on aluminum reveal that ultra-short pulses are the natural better solution for localizing energy in space and time for F～F _th. For higher fluences, pulses spread over tens of picoseconds and ended by a final peak enable a better impulsive coupling with the nascent plasma, optimizing its maximal temperature.     

Induced absorption in yttrium aluminium perovskite crystals irradiated by 12C and 235U ions

The present work is devoted to investigation of optical absorption in pure and neodymium-doped YAlO₃ (YAP) single crystals in the spectral range 0.2–1.1 μm induced by the influence of ¹²C ions irradiation with energy 4.50 MeV/u (MeV per nucleon) and a fluence 2 × 10⁹ cm^?2 or of ²³⁵U ion irradiation with energy 9.35 MeV/u and a fluence 5 × 10¹¹ cm^?2. The induced absorption in the case of ¹²C ions irradiation is caused by recharging of point growth defects and impurities under the radiation influence. After irradiation by ²³⁵U ions with fluence 5 × 10¹¹ cm^?2 the strong absorption rise is probably caused by contribution of the lattice destruction as a result of heavy ion bombardment.     

Electrode patterning on PEDOT:PSS thin films by pulsed ultraviolet laser for touch panel screens

Laser dry etching by a laser driven direct writing apparatus has been extensively used for the micro- and nano-patterning on the solid surface. The purpose of this study is to pattern the PEDOT:PSS thin film coated on the soda-lime glass substrates by a nano-second pulsed ultraviolet laser processing system. The patterned PEDOT:PSS film structure provides the electrical isolation and prevents the electrical contact from each region for capacitive touch screens. The surface morphology, geometric dimension, and edge quality of ablated area after the variety of laser patternings were measured by a 3D confocal laser scanning microscope. After the single pulse laser irradiation, the ablation threshold of the PEDOT:PSS film conducted by the nano-second pulsed UV laser was determined to be 0.135±0.003 J/cm². The single pulse laser interacted region and the ablated line depth increased with increasing the laser fluence. Moreover, the inner line width of ablated PEDOT:PSS films along the patterned line path increased with increasing the laser fluence but the shoulder width increased with decreasing fluence, respectively. The clean, smooth, and straight ablated edges were accomplished after the electrode patterning with the laser fluence of 1.7 J/cm² and 90 % overlapping rate.