Pulse laser ablation at water–air interface

We studied a new pulse laser ablation phenomenon on a liquid surface layer, which is caused by the difference between the refractive indices of the two materials involved. The present study was motivated by our previous study, which showed that laser ablation can occur at the interface between a transparent material and a gas or liquid medium when the laser pulse is focused through the transparent material. In this case, the ablation threshold fluence is reduced remarkably. In the present study, experiments were conducted in water and air in order to confirm this phenomenon for a combination of two fluid media with different refractive indices. This phenomenon was observed in detail by pulse laser shadowgraphy. A high-resolution film was used to record the phenomenon with a Nd:YAG pulse laser with 10-ns duration as a light source. The laser ablation phenomenon on the liquid surface layer caused by a focused Nd:YAG laser pulse with 1064-nm wavelength was found to be followed by the splashing of the liquid surface, inducing a liquid jet with many ligaments. The liquid jet extension velocity was around 1000 m/s in a typical case. The liquid jet decelerated drastically due to rapid atomization at the tips of the ligaments. The liquid jet phenomenon was found to depend on the pulse laser parameters such as the laser fluence on the liquid surface, laser energy, and laser beam pattern. The threshold laser fluence for the generation of a liquid jet was 20 J/cm². By increasing the incident laser energy with a fixed laser fluence, the laser focused area increased, which eventually led to an increase in the size of the plasma column. The larger the laser energy, the larger the jet size and the longer the temporal behavior. The laser beam pattern was found to have significant effects on the liquid jet’s velocity, shape, and history.     

Characterization of excimer laser ablation generated pepsin particles using multi-wavelength photoacoustic instrument

Preparation of organic thin layers on various special substrates using the pulsed laser deposition (PLD) technique is an important task from the point of view of bioengineering and biosensor technologies. Earlier studies demonstrated that particle ejection starts during the ablating laser pulse resulting in significant shielding effects which can influence the real fluence on the target surface and consequently the efficiency of layer preparation. In this study, we introduce a photoacoustic absorption measurement technique for in-situ characterization of ablated particles during PLD experiments. A KrF excimer laser beam (λ=248 nm, FWHM=18 ns) was focused onto pepsin targets in a PLD chamber; the applied laser fluences were 440 and 660 mJ/cm². We determined the wavelength dependence of optical absorption and mass specific absorption coefficient of laser ablation generated pepsin aerosols in the UV–VIS–NIR range. On the basis of our measurements, we calculated the absorbance at the ablating laser wavelength, too. We demonstrated that when the laser ablation generated pepsin aerosols spread through the whole PLD chamber the effect of absorptivity is negligible for the subsequent pulses. However, the interaction of the laser pulse and the just formed particle cloud generated by the same pulse is more significant.     

Aluminum thin film enhanced IR nanosecond laser-induced frontside etching of transparent materials

Laser processing of glass is of significant commercial interest for microfabrication of precision optical engineering devices. In this work, a laser ablation enhancement mechanism for microstructuring of glass materials is presented. The method consists of depositing a thin film of aluminum on the front surface of the glass material to be etched. The laser beam modifies the glass material by being incident on this front-side. The influence of ablation fluence in the nanosecond regime, in combination with the deposition of the aluminum layer of various thicknesses, is investigated by determining the ablation threshold for different glass materials including soda-lime, borosilicate, fused silica and sapphire. Experiments are performed using single laser pulse per shot in an air environment. The best enhancement in terms of threshold fluence reduction is obtained for a 16 nm thick aluminum layer where a reduction of two orders of magnitude in the ablation threshold fluence is observed for all the glass samples investigated in this work.     

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.     

Formation of microtower structures on nanosecond laser ablation of liquid metals

We report the formation of microtower structures, observed on multishot nanosecond laser irradiation of liquid metals (Ga, In, Sn–Pb alloy, Wood’s metal). Ablation in a reactive ambient gas (air, nitrogen, sulfur hexafluoride, nitrogen trifluoride) is shown to lead to a tower-like structure growing on the irradiated surface at a rate of 3–20 μm per pulse depending on laser fluence and the types of metal and ambient gas. The interplay between different processes in the heat-affected zone of the irradiated samples is analyzed, including ablation, thermal expansion, temperature variations of viscosity, surface tension, thermal stresses, capillary effects, and surface chemistry. A clear picture of microtower origin has been established, and qualitative modeling can explain the formation mechanism.     

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.     

Laser-assisted generation of self-assembled microstructures on stainless steel

Utilising a Nd:YVO₄ laser (wavelength of 532 nm, pulse duration of 8 ns, repetition rate of 30 kHz) and a Nd:YAG laser (wavelength of 1064 nm, pulse duration of 7 ns, repetition rate of 25 kHz), it was found that during the pulsed laser ablation of metal targets, such as stainless steel, periodic nodular microstructures (microcones) with average periods ranging from ∼30 to ∼50 μm were formed. This period depends on the number of accumulated laser pulses and is independent of the laser wavelength. It was found that the formation of microcones could occur after as little as 1500 pulses/spot (a lower number than previously reported) are fired onto a target surface location at laser fluence of ∼12 J/cm², intensity of ∼1.5 GW/cm². The initial feedback mechanism required for the formation of structures is attributed to the hydrodynamic instabilities of the melt. In addition to this, it has been shown that the structures grow along the optical axis of the incoming laser radiation. We demonstrate that highly regular structures can be produced at various angles, something not satisfactorily presented on metallic surfaces previously. The affecting factors such as incident angle of the laser beam and the structures that can be formed when varying the manner in which the laser beam is scanned over the target surface have also been investigated.     

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     

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.     

Time-resolved shock-wave photography above 193-nm excimer laser-ablated graphite surface

Highly oriented pyrolytic graphite (HOPG) was ablated by a 193-nm ArF excimer laser in air. The fluence was varied in the range 1-25 J/cm². Every laser shot hit a pristine graphite surface. The emerging shock wave was recorded by a nanosecond-resolution photographic arrangement. The velocity of the shock wave as a function of time and laser fluence was measured. The amount of energy that generates the shock wave was determined and found to be about 5-7% of the incident laser energy. The shock wave is already present 10-15 ns after the maximum of the incident laser pulse. These facts imply that, even if high-energy (10-100 eV) ions, atoms, or clusters leave the surface, a layer several 10 nm thick has to be removed during this short period. The temperature of the shock front is ~2500-4000 K, as derived from the measured velocities. Measuring the ablation depth by atomic force microscopy as a function of fluence revealed that the single-shot ablation threshold is 1.4ǂ.2 J/cm², and the effective absorption coefficient is ~1.5᎒⁵ cm^-1.     

Optical transmission and reflection of aluminum film irradiated by nanosecond laser beam and experimental studying of phase-explosion

In this paper we present evidence for a phase explosion during the laser-induced ablation process by studying the optical reflectivity of the ablated plume. The ablation was produced by irradiating thin film aluminum coated on a quartz substrate with a single pulse laser beam in ambient air. The laser pulse was provided by the second harmonic of a Q-switched Nd:YAG laser with ∼10 ns pulse duration. The transmission of a low power He–Ne laser beam through the hot ablated material plume and its reflection (from the front surface, and rear surface of aluminum film) were also monitored during the duration of the ablation event. The results show that the front surface reflectivity is enhanced at an early time of ablation which is described as strong evidence for the creation of a phase explosion in this process.     

Formation of cavitation-induced pits on target surface in liquid-phase laser ablation

It is well known that a crater is formed on the target surface by the irradiation of intense laser pulses in laser ablation. In this work, we report that additional pits are formed on the bottom surface of the ablation crater due to the collapse of a cavitation bubble in liquid-phase laser ablation. We observed the formation of several cavitation-induced pits when the fluence of the laser pulse used for ablation was approximately 5 J/cm². The number of cavitation-induced pits decreased with the laser fluence, and we observed one or two cavitation-induced pits when the laser fluence was higher than 10 J/cm². In addition, we examined the influence of the liquid temperature on the formation of cavitation-induced pits. The collapse of the cavitation bubble was not observed when the liquid temperature was close to the boiling temperature, and in this case, we found no cavitation-induced pits on the bottom surface of the ablation crater. This experimental result was discussed by considering the cavitation parameter.     

Deep drilling on a silicon plate with a femtosecond laser: experiment and model analysis

The ablation rate when drilling fine holes having large aspect ratios in silicon substrates with femtosecond laser pulses was estimated from mechanically ground cross sections of the ablated holes. The ablation rate shows a dramatic change at the depth at which the laser pulse reaches a certain fluence, which is nearly constant when the initial laser fluence was varied from 14.5 to 59.4 J/cm². The ablation rate, threshold fluence, in three fluence domains, and the transition fluences at which the ablation rate shows a dramatic change, were derived. However, when a pulse energy of 200 μJ was used a much greater ablation rate was obtained, suggesting that another fluence domain for larger ablation rates exists. The experimentally obtained hole depths as a function of shot numbers were reproduced by a theoretical model, which incorporates laser pulse attenuation in the holes that is the same as that in waveguides for some attenuation coefficient and ablation rates for three fluence domains. PACS 42.62.-b; 42.65.Re; 78.40.Fy; 78.47.+p; 81.20.Wk     

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.      

XPS studies of short pulse laser interaction with copper

The effect of laser ablation on copper foil irradiated by a short 30 ns laser pulse was investigated by X-ray photoelectron spectroscopy. The laser fluence was varied from 8 to 16.5 J/cm² and the velocity of the laser beam from 10 to 100 mm/s. This range of laser fluence is characterized by a different intensity of laser ablation. The experiments were done in two kinds of ambient atmosphere: air and argon jet gas.The chemical state and composition of the irradiated copper surface were determined using the modified Auger parameter (α′) and O/Cu intensity ratio. The ablation atmosphere was found to influence the size and chemical state of the copper particles deposited from the vapor plume. During irradiation in air atmosphere the copper nanoparticles react with oxygen and water vapor from the air and are deposited in the form of a CuO and Cu(OH)₂ thin film. In argon atmosphere the processed copper surface is oxidized after exposure to air.     

Nanosecond pulsed laser ablation of silicon in liquids

Laser fluence and laser shot number are important parameters for pulse laser based micromachining of silicon in liquids. This paper presents laser-induced ablation of silicon in liquids of the dimethyl sulfoxide (DMSO) and the water at different applied laser fluence levels and laser shot numbers. The experimental results are conducted using 15 ns pulsed laser irradiation at 532 nm. The silicon surface morphology of the irradiated spots has an appearance as one can see in porous formation. The surface morphology exhibits a large number of cavities which indicates as bubble nucleation sites. The observed surface morphology shows that the explosive melt expulsion could be a dominant process for the laser ablation of silicon in liquids using nanosecond pulsed laser irradiation at 532 nm. Silicon surface’s ablated diameter growth was measured at different applied laser fluences and shot numbers in both liquid interfaces. A theoretical analysis suggested investigating silicon surface etching in liquid by intense multiple nanosecond laser pulses. It has been assumed that the nanosecond pulsed laser-induced silicon surface modification is due to the process of explosive melt expulsion under the action of the confined plasma-induced pressure or shock wave trapped between the silicon target and the overlying liquid. This analysis allows us to determine the effective lateral interaction zone of ablated solid target related to nanosecond pulsed laser illumination. The theoretical analysis is found in excellent agreement with the experimental measurements of silicon ablated diameter growth in the DMSO and the water interfaces. Multiple-shot laser ablation threshold of silicon is determined. Pulsed energy accumulation model is used to obtain the single-shot ablation threshold of silicon. The smaller ablation threshold value is found in the DMSO, and the incubation effect is also found to be absent.     

Non-contact acoustic tests based on nanosecond laser ablation: Generation of a pulse sound source with a small amplitude

A method to generate a pulse sound source for acoustic tests based on nanosecond laser ablation with a plasma plume is discussed. Irradiating a solid surface with a laser beam expands a high-temperature plasma plume composed of free electrons, ionized atoms, etc. at a high velocity throughout ambient air. The shockwave generated by the plasma plume becomes the pulse sound source. A laser ablation sound source has two features. Because laser ablation is induced when the laser fluence reaches 10¹²–10¹⁴ W/m², which is less than that for laser-induced breakdown (10¹⁵ W/m²), laser ablation can generate a lower sound pressure, and the sound source has a hemispherical radiation pattern on the surface where laser ablation is generated. Additionally, another feature is that laser-induced breakdown sound sources can fluctuate, whereas laser ablation sound sources do not because laser ablation is produced at a laser beam–irradiation point. We validate this laser ablation method for acoustic tests by comparing the measured and theoretical resonant frequencies of an impedance tube.     

Enhancement of resolution and quality of nano-hole structure on GaN substrates using the second-harmonic beam of near-infrared femtosecond laser

By using a second harmonic of near infrared femtosecond (fs) laser (λ=387 nm, 150 fs) with high NA objective lens, fabrication resolution has been greatly improved in nano-fabrication of wide band-gap semiconductor gallium nitride (GaN). We have carried out a wet-chemical-assisted fs laser ablation method, in which the laser beam is focused onto a single-crystal GaN substrate immersed in a concentrated hydrochloric (HCl) acid solution. A two-step processing involving irradiation with a fs laser beam in air followed by wet chemical treatment is also performed for comparison. In the wet-chemical-assisted ablation, theoretical diameters of ablation craters are calculated as a function of pulse energy by assuming that the reaction is based on two-photon absorption. In lower energy, the calculated curve is close to the experimental value, while the actual measured diameters in the region of higher energy are larger than calculated values. In the condition of the highest fabrication resolution, we obtained ablation craters smaller than 200 nm at full width at half maximum. We have also demonstrated the fabrication of two-dimensional (2D) periodic nanostructures on surface of a GaN substrate using the second harmonic single fs-laser pulse. Uniform ablation craters with the size as small as 410 nm in diameter are arranged with a periodicity of 1 μm. Such structures are applicable to 2D photonic crystals which improve the light extraction efficiency for blue LEDs in the near future.     

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.     

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.