Material processing of dielectrics with temporally asymmetric shaped femtosecond laser pulses on the nanometer scale

Laser material processing of dielectrics with temporally asymmetric femtosecond laser pulses of identical fluence, spectrum, and statistical pulse duration is investigated experimentally. To that end single shot structures at the surface of fused silica as a function of fluence and pulse shape are analyzed with the help of scanning electron microscopy. Structures for the bandwidth limited pulses show the known expansion in structure size with increasing laser fluence approaching the diffraction limit, which is 1.4 μm for the 0.5NA microscope objective used. In contrast, structures from the asymmetric pulses are remarkably stable with respect to variations in laser fluence and stay below 300 nm despite doubling the fluence. Different thresholds for surface material modification with respect to an asymmetric pulse and its time reversed counterpart are attributed to control of different ionization processes.     

Combined continuum-atomistic modeling of ultrashort-pulsed laser irradiation of silicon

Ultrafast thermomechanical responses of silicon thin films due to ultrashort-pulsed laser irradiation were investigated using an atomic-level hybrid method coupling the molecular dynamics and the ultrafast two-step energy transport model. The dynamic reflectivity and absorption were considered, and the effects of laser fluence and pulse duration on the thermomechanical response were studied. It was found that both the carrier temperature and number density rapidly increase to their maximum while the lattice temperature rises at a much slower rate. The ultrafast laser heating could induce a strong stress wave in the film, with the maximum compressive and tensile stress occurring near the front and back surfaces, respectively. For laser pulses of the same duration, the higher the laser fluence is, the higher the carrier temperature and density and lattice temperature are induced. For the same laser fluence, a longer pulse generally produces lower carrier density and temperatures and weaker stress shock strength. However, for the fluence of 0.2 J/cm², the lowest lattice temperature was simulated for a 100-fs pulse compared to the 1-ps and 5-ps pulses, due to the increase of reflectivity by high carrier density. It is also shown that the optical properties as functions of lattice temperature usually employed are not suited for modeling ultrafast laser interactions with silicon materials.     

Morphology and composition on Al surface irradiated by femtosecond laser pulses

We study the surface chemicals and structures of aluminum plates irradiated by scanning femtosecond laser pulses in air for a wide range of laser fluence from 0.38 to 33.6 J/cm². X-ray photoelectron spectroscopy and X-ray diffraction analyses indicate clearly that crystalline anorthic Al(OH)₃ is formed under femtosecond laser pulse irradiation. Besides aluminum hydroxide, crystalline Al₂O₃ is also found in the samples irradiated at high laser fluence. Field emission scanning electron microscopy demonstrates that the surfaces of the samples irradiated with low laser fluence are colloidal-like and that nanoparticles with a few nanometers in size are embedded in glue-like substances. For high laser fluence irradiated samples, the surfaces are highly porous and covered by nanoparticles with uniform size of less than 20 nm.     

Sub-surface damage in indium phosphide caused by micromachining of grooves with femtosecond and nanosecond laser pulses

Grooves laser-micromachined in InP using 130 fs and 8 ns pulses with fluences 2 and 0.7 J/cm² are investigated by cross-sectional transmission electron microscopy. At the fluence of 2 J/cm², irradiation with both femtosecond and nanosecond laser pulses yield substantial resolidified layers with a maximum thickness of 0.5 m. In contrast, at the fluence of 0.7 J/cm², irradiation with nanosecond pulses leads to a layer of similar thickness, while femtosecond irradiation produces laser induced periodic surface structures with minimal resolidified material. For both fluences, femtosecond pulses generate substantial densities of defects extending over a few microns in depth, while nanosecond laser irradiation leads to no observable damage beneath the resolidified layer. The high peak power density and the stress confinement obtained from femtosecond pulses, along with incubation effects, are identified as the major factors leading the observed plastic deformations. PACS 61.80.Ba; 68.35.Gy; 79.20.Ds     

Nonlinear photoionization in the soft X-ray regime

We present the results of 800 and 400 nm wavelength, femtosecond laser pulse irradiation of a sample consisting of a metal film on thermally-grown oxide on silicon. On selected sites, cross-sectional transmission electron microscopy was performed to provide information on sub-surface changes not observable with surface scanning electron microscopy. A range of pulse energies in single-pulse irradiation exists for which the metal film was removed but the oxide was not appreciably thinned. For a sufficiently high pulse energy within this range, substantial defects were observed in the underlying silicon. Five infrared pulses of a relatively high fluence created significant defects, as well as producing polycrystalline material on top of the original oxide and metal. We discuss various factors which may play a role in the formation of the observed features. PACS 61.72.Ff; 68.37.Lp; 79.20.Ds     

Acoustic superscatterer and its multilayer realization

Picosecond (40 ps) pulsed Nd:YAG laser irradiation of a WTi thin film on silicon with a wavelength of 532 nm and a fluence 2.1 J/cm² was performed in air. This led to significant changes of the chemical composition and morphology on the surface of the WTi thin film. The results show an increase in surface roughness, due to formation of conical structures, about 50 nm wide in the base, and a very thin oxide layer composed of WO₃ and TiO₂, with a dominant TiO₂ phase at the top, within the depth of about 20 nm. The thickness of the oxide layer was dependent on the number of laser pulses. The samples were analyzed by scanning electron microscopy, atomic force microscopy, and X-ray photoelectron spectroscopy.     

Effects of laser pulse heating of copper photocathodes on high-brightness electron beam production at blowout regime

Producing high-brightness and high-charge(100 pC) electron bunches at blowout regime requires ultrashort laser pulses with high fluence. The effects of laser pulse heating of the copper photocathode are analyzed in this paper. The electron and lattice temperature is calculated using an improved two-temperature model, and an extended Dowell-Schmerge model is employed to calculate the thermal emittance and quantum efficiency. A timedependent growth of the thermal emittance and the quantum efficiency is observed. For a fixed amount of charge,the projected thermal emittance increases with decreasing laser radius, and this effect should be taken into account in laser optimization at blowout regime. Moreover, laser damage threshold fluence is simulated, showing that the maximum local fluence should be less than 40 mJ/cm~2 to prevent damage to the cathode.     

Fabrication and sub-band-gap absorption of single-crystal Si supersaturated with Se by pulsed laser mixing

Selenium supersaturated silicon layers were fabricated by pulsed excimer laser induced liquid-phase mixing of thin Se films on Si(001) wafers. Sufficiently low Se coverage avoids destabilization of rapid epitaxial solidification, resulting in supersaturated solid solutions free of extended defects, as shown by transmission electron microscopy. The amount of retained Se depends on the original film thickness, the laser fluence, and the number of laser pulses irradiating the same spot on the surface. Using this method, Se has incorporated into the topmost 300 nm of the silicon with a concentration of 0.1 at.%. Channeling Rutherford backscattering spectrometry measurements show that the substitutional fraction can be as high as 75% of the total retained Se. These alloys exhibit strong sub-band-gap absorption with optical absorption coefficient ranging up to about 10⁴ cm⁻¹, thus making them potential candidates for applications in Si-based optoelectronic devices.     

Laser-reactive ablation deposition of silicon-nitride films

Silicon-nitride films were deposited on silicon waters by XeCl (308 nm) excimer-laser ablation of silicon in low-pressure (0.05–5 mbar) ammonia atmospheres. Series of 10 000 pulses at the repetition rate of 8 Hz were directed to the target surface. The fluence was set at about 5 J/cm². Pulse duration was about 30 ns. The deposited films were characterized by different techniques (X-ray diffraction, X-ray photoelectron spectroscopy, Auger electron spectroscopy, Rutherford backscattering spectrometry, scanning electron microscopy, profilometry). Silicon-nitride films with thickness close to 1 m were obtained under specific experimental conditions.     

Sub-picosecond ultraviolet laser filamentation-induced bulk modifications in fused silica

We present experiments with sub-picosecond ultraviolet laser pulses (248 nm, 450 fs) tightly focused in the bulk of fused-silica samples. The high laser intensities attained generate plasma through multi-photon absorption and electron avalanche processes in the bulk of the material. Depending on the initial experimental conditions three distinct types of structural changes in the material are observed, from small changes of the refractive index to birefringence, and even cracks and voids. We also observe the creation of micro-channels, up to 115 m in length, inside the material due to self-guiding and filamentation of the laser pulses in the transparent material. The selective change of the refractive index is a promising method for the fabrication of photonic structures such as waveguides and three-dimensional integrated optical devices. PACS  52.38.Hb; 42.65.-k; 42.70.-a     

Laser machining of silicon nitride based composite cantilever structures

Cantilever structures from silicon nitride based composite ceramic materials were produced using laser cutting. A picosecond laser was used to cut two-dimensional meso sized cantilever structures up to 450 μm thickness in conductive and insulating ceramics. A practical experimental based approach was used, where various parameters of the laser cutting process were altered to produce a cut surface with a damage zone of 5–10 μm. The quality of the cut ceramics was investigated by optical and scanning electron microscopy. The results are presented along with the properties of the laser cut surface, including the damage zone, formation of cracks and the reaction products.     

Incubation/ablation patterning of polymer surfaces with sub-μm edge definition for optical storage devices

By exposure to low fluence UV laser radiation, the optical absorption coefficient of subsurface polymer material can be increased (incubation) with spatial control, using a suitable contact mask, proper imaging of the mask, or laser direct writing. Spatially selective ablation of polymethylmethacrylate (PMMA) is then achieved with large area XeCl excimer laser pulses at 308 nm. In this way, the transfer of spatial information to the material can be decoupled from the high laser fluence removal (ablation) step. The advantages are: The mask is exposed to only low fluence laser radiation — damage is avoided. Since the mask can be removed before the ablation step, mask contamination by the ablated plume cannot occur. Using this incubation/ablation method, PMMA surfaces can be patterned (248 nm/308 nm) with submicrometer spatial control and edge contrasts better than 0.2 m. This has impact on optical storage technology and laser surface processing techniques in general. The smallest single structure obtained was somewhat smaller than 0.5 m in diameter up to now, given by the mask.Presented at Laserion '91, June 12–14, 1991     

Projection ablation of glass-based single and arrayed microstructures using excimer laser

Ablation of single and arrayed microstructures using an excimer laser is studied. The single feature microstructures are fabricated for evaluating the ablation mechanism, threshold fluence, and associated material removing (ablation) rate. The morphology changes during ablation are investigated with the focus on the formation of the ablation defects, debris or recast. The possibility of removing these defects is also evaluated and demonstrated. The present study concentrates on the borosilicate glass, although ablation of polyimide and silicon are performed and discussed for comparison. Polyimide and silicon are the most popular polymer or semiconductor material used in the electronics industry. The arrayed microstructures are ablated to demonstrate the fact that, by repetition of a simple-patterned mask associated with synchronized laser pulses and substrate movement, arrayed and more complex structures can be cost-effectively manufactured. The potential applications of these arrayed microstructures are discussed and illustrated. A low-cost replication technique that uses the arrayed microstructure presently machined as the forming mold for making electroforming nickel microneedles is specifically presented. Finally, the potential areas of using excimer laser in micromachining of glass-based structures for future research are also briefly covered.     

Tungsten silicide formation by XeCl excimer-laser irradiation of W/Si samples

We report a study of the formation of tungsten silicide at the W-Si interface, induced by multipulse (up to 300 shots) XeCl excimer-laser irradiation of W(150 nm)/Si and W(500 nm)/Si samples. Laser fluences ranging from 0.6 to 1.8 J/cm² were used. After laser treatment the samples were examined by different diagnostic techniques: Rutherford backscattering spectrometry, X-ray scattering, resistometry, and surface profilometry. Numerical computations of the evolution and depth profiles of the temperature in the samples as a consequence of a single 30 ns laser pulse were performed as well. The results indicate that it is possible to obtain a tungsten silicide layer at the W-Si interface at quite low fluences. The layer thickness increases with the number of laser pulses. Complete reaction of the 150 nm thick W film with silicon was obtained at the fluence of 1.2 J/cm² between 30 and 100 laser pulses and at 1.5 J/cm² after 30 laser pulses. The sheet resistance of these silicides was 5–10 . At the used fluences for the 500 nm thick W film only the onset of silicide synthesis at the W-Si interface was observed.     

Femtosecond laser-induced damage morphologies of crystalline silicon by sub-threshold pulses

The effect of sub-threshold pulses of circularly polarized Ti:sapphire femtosecond laser system on crystalline (1 0 0) silicon wafer was investigated. Surface damage morphologies were studied by irradiating the test silicon surface with pulses (peak fluence of 0.25 J/cm²) in succession. These pulses were below the single-pulse surface damage threshold. After the few initial pulses, the observed surface damage morphologies were found to be characterized by a minor phase change region and a major surface damage area at the center, corresponding to the well-known laser-induced periodic surface structure (LIPSS). Further increase in the number of pulses resulted in the formation of new surface morphologies with different features such as ablation, modification, and re-deposited materials. These features were reproducible and more distinguishable at higher number of pulses.     

Single- and multi-pulse formation of surface structures under static femtosecond irradiation

Femtosecond surface structure modifications are investigated under irradiation with laser pulses of 150 fs at 800 nm, on copper and silicon. We report sub-wavelength periodic structures formation (ripples) with a periodicity of 500 nm for both materials. These ripples are perpendicular to the laser polarization and can be obtained with only one pulse. The formation of these ripples corresponds to a fluence threshold of 1 J/cm² for copper and 0.15 J/cm² for silicon. We find several morphologies when more pulses are applied: larger ripples parallel to the polarization are formed with a periodicity of 1 μm and degenerate into a worm-like morphology with a higher number of pulses. In addition, walls of deep holes also show sub-wavelength and large ripples.     

Studies on excimer laser doping of GaAs using sulphur adsorbate as dopant source

Excimer laser doping of GaAs using sulphur adsorbate as a dopant source is demonstrated. Box-like n-type layers of depths of about 100 nm with carrier concentration as high as (23)×10¹⁹ cm^–3 are formed. Passivation of GaAs using a (NH₄)₂S_x solution for 40 min followed by sublimation of the excess sulphur atoms in high vacuum result in an effective dopant for controllable n-type doping. The samples are irradiated using a KrF excimer laser in a N₂ gaseous environment. Secondary ion mass spectrometry (SIMS) measurements show that sulphur is successfully incorporated in the GaAs. The sheet resistance is controlled by adjusting the laser energy fluence and number of laser pulses. Rutherford backscattering spectrometry with channeling (RBS/C) alignment measurement indicates that lattice damage is undetectable for N₂ gas pressures of 760 Torr.     

KrF laser ablation of a polyethersulfone film: Effect of pulse duration on structure formation

Polyethersulfone (PES) films were processed with KrF laser irradiation of different pulse durations (τ). Scanning electron microscopy (SEM) and Raman spectroscopy were employed for the examination of the morphology and chemical composition of the irradiated surfaces, respectively. During ablation with 500 fs and 5 ps pulses, localized deformations (beads), micro-ripple and conical structures were observed on the surface depending on the irradiation fluence (F) and the number of pulses (N). In addition, the number density of the structures is affected by the irradiation parameters (τ, F, N). Furthermore, at longer pulse durations (τ = 30 ns), conical structures appear at lower laser fluence values, which are converted into columnar structures upon irradiation at higher fluences. The Raman spectra collected from the top of the structures following irradiation at different pulse durations revealed graphitization of the ns laser treated areas, in contrast to those processed with ultra-short laser pulses.     

Excimer laser projection micromachined free-standing polymer films

Projection etching techniques using 308 nm and 248 nm excimer laser illumination have been investigated as a means of micromachining thin free-standing polymer films. Consideration is given to the choice of operating parameters (wavelength, fluence) to minimise damage to the machined structures. High quality grid patterns have been produced on free-standing mylar films with a thickness down to 1.5 μm.