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.     

Surface modifications of materials by repetitive laser pulses

Laser-induced modifications on platinum (Pt) and silicon (Si) are compared by considering the development of various features on the irradiated surface. The experiments were carried out both in air and under vacuum. The interaction of 50 pulses of 1064 nm Nd:YAG laser with both targets in air resulted in non-linear phenomena. The periphery of the irradiated spot on the Pt surface exhibits wave-like patterns with a featureless central portion. A non-uniform distribution of cones of different sizes is also observed on the irradiated surface. In the case of silicon, the laser-induced periodic surface structures along with the formation of micro-column, rectangular blocks and grid are prominently observed features. However, when both the targets were irradiated with the same number of shots under vacuum (～10^?3 Torr), the surface morphologies of both the targets exhibited the hydrodynamic sputtering but with more explosive expulsion in Pt when compared with silicon. In platinum, there is a periodic variation in the distance between adjacent cones formed in various ablated zones. The Gaussian beam mode TEM₀₀ provided the evidences for melt pool formation in silicon when irradiated under vacuum. Additionally, we observed other mechanisms including splashing, sputtering, burning, re-solidification and redeposition on the surface of irradiated targets.     

STEM (scanning transmission electron microscopy) analysis of femtosecond laser pulse induced damage to bulk silicon

This work reports on the structural changes that take place in wafer grade silicon when it is micro-machined with ultra-short laser pulses of 150 fs duration. A Chirped Pulse Amplification (CPA) Ti:Sapphire laser was used, with an operating wavelength centered on 775 nm and a maximum repetition rate of 1 KHz. The laser induced damage was characterized over the fluence range 0.43–14 Jcm^-2, and for each fluence a progressively increasing number of pulses was used. The analytical tools used to characterize the samples were all based upon electron microscopy. A 30 KeV scanning transmission electron microscope (STEM) imaging technique was developed to observe defects in the crystal lattice and the thermal-mechanical damage in the area surrounding the laser machined region. Mechanical cross sectioning (in conjunction with Scanning Electron Microscope (SEM) surface imaging) was also used to reveal the internal structure, composition, and dimensions of the laser machined structures. Based on this analysis, it will be shown that laser machining of silicon with femtosecond pulses can produce features with minimal thermal damage, although lattice damage created by mechanical stresses and the deposition of ablated material both limit the extent to which this can be achieved, particularly with high aspect ratios. A key feature of the work presented here is the high-resolution STEM images of the laser-machined structures. PACS  42.65.Re; 42.62.Cf; 61.80.Ba; 61.82.Fk; 68.37.Hk; 68.37.Lp     

Accumulation morphology on the surface of stainless steel irradiated by a nanosecond Nd:YAG pulsed laser

In this study, results in the irradiation of stainless steel AISI 304 in air with nanosecond laser pulses at laser irradiation power density 4×10⁷ W/cm² are reported. Laser processing parameters, such as wavelengths 532 and 1064 nm, pulse duration 20 ns and repetition rate 10 Hz were used. It is shown that the surface morphology of the stainless steel is related to the number of pulses applied to the same spot. The following surface morphological changes were observed: (i) occurrence of the micro-grains microstructures at wavelengths 532 and 1064 nm after 10 000 pulses irradiation and (ii) occurrence of vermiform-like microstructures at wavelength 1064 nm after 1000 pulses irradiation. Generally, it is concluded that irradiation due to several consecutive pulses caused significant damage and enhanced the stainless steel surface roughness.     

Multipulse irradiation of silicon by femtosecond laser pulses: Variation of surface morphology

The multipulse interaction of ultraviolet femtosecond laser pulses with silicon and generation of surface structures in a large area spot (?1 mm²) has been studied. The evolution of multiscale structures at the constant fluence strongly depends on the number of pulses, N. For N < 200, the “carpet-like” pattern of nano-, and micro-spikes is generated by the bubble explosion in a thin surface foam layer. The accumulation of bubbles and their explosion due to repetition of laser pulses cause damped membrane-like oscillations of the silicon surface. For 200 ≤ N, bifurcation of surface morphology takes place: (i) the surface tension waves of the wavelength ∼200 μm appear in the peripheral region of the spot. Generated by the surface thermal gradient in the liquid foam layer, they spread from the hot centerline towards the periphery of the spot. The change of their wavelength with propagation distance indicates onset of the Eckhaus instability caused by the phase modulation in multipulse interaction. (ii) Deep caverns appear in a highly superheated silicon layer in the central region of the spot due to the fast gas-liquid phase separation and the fragmentation process.     

Recrystallization of germanium surfaces by femtosecond laser pulses

The damage morphology of germanium surfaces using femtosecond laser pulses of various fluences and number of pulses is reported. The single pulse damage threshold in the present experiment was 9.7±4.0×10⁻¹³ W/cm². The experimental threshold value was compared with theory, considering the damage threshold as the melting threshold. The cooling rate calculated on the basis of present results is 2.4×10^15°C/s. Recrystallization was the common feature of the damage morphology. For fluences greater than the single pulse damage-threshold micropits and spherical grains of micron size were formed in the damaged surface. Ablation (surface removal) was also observed at higher fluences (at two or three times of damage threshold value). The damage morphology, induced by multiple pulses, was unaffected for linear and circular polarization.     

Surface damage morphology investigations of silicon under millisecond laser irradiation

The surface damage morphologies of single crystal silicon induced by 1064 nm millisecond Nd:YAG laser are investigated. After irradiation, the damage morphologies of silicon are inspected by optical microscope (OM) and atomic force microscope (AFM). The plasma emission spectra of the damaged region are detected by the spectrometer. It is shown that surface oxidation and nitridation have occurred during the interaction of millisecond laser with silicon. In addition, the damage morphologies induced by 2 ms and 10 ns pulse width laser are compared. The damage morphology obtained by 2 ms laser is an evident crater. Three types of damage morphologies are formed at different laser energy densities. The circular concentric ripples are found surrounding the rim of the crater. The spacing of the ripples is 15 ± 5 μm. Two types of cracks are observed: linear crack and circular crack. The linear crack is observed in the center of the damaged region which propagates to the periphery of the damaged region. The circular crack is located at the rim of the crater. The damage morphology induced by 10 ns laser is surface layer damage. The periodic linear waves are generated due to the interference between the incident beam and the scattered beam. The spacing of the ripples is 1.54 μm which is close to the incident laser wavelength 1.064 μm. The linear crack is located at the center of the damaged region. Furthermore, for the same laser energy density, the dimension of the damaged region and the crater depth induced by 2 ms laser are greater than that of 10 ns laser. It indicates that the damage mechanism under millisecond pulse laser irradiation is strongly different from the case of nanosecond pulse laser.     

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.     

Plasmonic laser nanoablation of silicon by the scattering of femtosecond pulses near gold nanospheres

We present the fabrication of nanostructures ablated on silicon(100) by the plasmonic scattering of 780 nm, 220 fs laser pulses in the near-field of gold nanospheres. We take advantage of the enhanced plasmonic scattering of ultrashort laser light in the particle near-field to ablate well-defined nanocraters. Gold nanospheres of 150 nm diameter are deposited onto a silicon surface and irradiated with a single laser pulse. We studied the effect of laser polarization on the morphology of ablated nanostructures and estimated the minimum fluence for plasmonic nanoablation. When the polarization of the incident radiation is directed at a 45° angle into the substrate surface, a near-field enhancement of 23.1±7.6 is measured, reducing the required silicon ablation fluence from 191±14 mJ/cm² to 8.2±2.9 mJ/cm². Enhancements are also measured for laser polarizations parallel to the substrate surface when the substrate is angled 0° and 45° to the incident irradiation, giving enhancements of 6.9±0.6 and 4.1±1.3, respectively. Generated nanocrater morphologies show a direct imprint of the particle dipolar scattering region, as predicted in our theoretical calculations. The measured near-field enhancement values agree well with the maximum field enhancements obtained in our calculations. The agreement between theory and measurements supports that the nanocraters are indeed formed by the enhanced plasmonic scattering in the near-field of the nanoparticles. PACS 42.62.-b; 52.38.Mf; 81.65.Cf; 81.16.-c; 78.67.Bf     

Comparing study of subpicosecond and nanosecond wet etching of fused silica

The effectiveness of the laser induced backside wet etching (LIBWE) of fused silica produced by subpicosecond (600 fs) and nanosecond (30 ns) KrF excimer laser pulses (248 nm) was studied. Fused silica plates were the transparent targets, and naphthalene-methyl-methacrylate (c = 0.85, 1.71 M) and pyrene-acetone (c = 0.4 M) solutions were used as liquid absorbents. We did not observe etching using 600 fs laser pulses, in contrast with the experiments at 30 ns, where etched holes were found. The threshold fluences of the LIBWE at nanosecond pulses were found to be in the range of 360-450 mJ cm⁻² depending on the liquid absorbers and their concentrations. On the basis of the earlier results the LIBWE procedure can be explain by the thermal heating of the quartz target and the high-pressure bubble formation in the liquid. According to the theories, these bubbles hit and damage the fused silica surface. The pressure on the irradiated quartz can be derived from the snapshots of the originating and expanding bubbles recorded by fast photographic setup. We found that the bubble pressure at 460 mJ cm⁻² fluence value was independent of the pulse duration (600 fs and 30 ns) using pyrene-acetone solution, while using naphthalene-methyl-methacrylate solutions this pressure was 4, 5 times higher at 30 ns pulses than it was at 600 fs pulses. According to the earlier studies, this result refers to that the pressure should be sufficiently high to remove a thin layer from the quartz surface using pyrene-acetone solution. These facts show that the thermal and chemical phenomena in addition to the mechanical effects also play important role in the LIBWE procedure.     

Sunlight loss for femtosecond microstructured silicon with two impurity bands

Black silicon,produced by irradiating the surface of a silicon wafer with femtosecond laser pulses in the presence of a sulfur-bearing gas,is widely believed to be a potential material for efficient multi-intermediate-band silicon solar cells.Taking chalcogen as an example,we analyse the loss of sunlight for silicon with two impurity bands and we find that loss of the sunlight can be minimized to 0.332 when Te 0 (0.307 eV) and Te + (0.411 eV) are doped into microstructured silicon.Finally,problems needed to be resolved in analysing the relationship between conversion efficiency of the ideal four-band silicon solar cell and the position of the introduced two intermediated bands in silicon according to detailed balance theory are pointed out with great emphasis.     

Synthesis by pulsed laser ablation in Ar and SERS activity of silver thin films with controlled nanostructure

Thin silver films were deposited by pulsed laser ablation in a controlled Ar atmosphere and their SERS activity was investigated. The samples were grown at Ar pressures between 10 and 70 Pa and at different laser pulse numbers. Other deposition parameters such as laser fluence, target to substrate distance and substrate temperature were kept fixed at 2.0 J/cm², 35 mm and 297 K. Film morphologies were investigated by scanning and transmission electron microscopies (SEM, TEM). Surface features range from isolated nearly spherical nanoparticles to larger islands with smoothed edges. Cluster growth is favored by plume confinement induced by background gas. After landing on the substrate clusters start to aggregate giving rise to larger structures as long as the deposition goes on. Such a path of film growth allows controlling the surface morphology as a function of laser pulse number and Ar pressure. These two easy-to-manage process parameters control the number density and the average size of the as-deposited nanoparticles. We investigated the influence of substrate morphologies on their surface enhanced Raman scattering properties. Raman measurements were performed after soaking the samples in rhodamine 6G aqueous solutions over the concentration range between 1.0 × 10⁻⁴ and 5.0 × 10⁻⁸ M. The sensitivity of the film SERS activity on the surface features is put into evidence.     

Evolution of InP surfaces under low fluence pulsed UV irradiation

An InP wafer was irradiated in air by a series of UV pulses from a nitrogen laser with fluences of 120 mJ/cm² and 80 mJ/cm². These fluences are below the single-pulse ablation threshold of InP. Over the studied region the distribution of the radiation intensity was uniform. The number of pulses varied from 50 to 6000. The evolution of the surface morphology and structure was characterized by atomic force microscopy, optical microscopy and Raman spectroscopy. The relationship between mound size and the number of pulses starts out following a power law, but saturates for a sufficiently high number of pulses. The crossover point is a function of fluence. A similar relation exists for the surface roughness. Raman spectroscopic investigations showed little change in local crystalline structure of the processed surface layer.     

Nanosecond laser damage resistance of differently prepared semi-finished parts of optical multimode fibers

Optical multimode fibers are applied in materials processing (e.g. automotive industry), defense, aviation technology, medicine and biotechnology. One challenging task concerning the production of multimode fibers is the enhancement of laser-induced damage thresholds. A higher damage threshold enables a higher transmitted average power at a given fiber diameter or the same power inside a thinner fiber to obtain smaller focus spots.In principle, different material parameters affect the damage threshold. Besides the quality of the preform bulk material itself, the drawing process during the production of the fiber and the preparation of the fiber end surfaces influence the resistance. Therefore, the change of the laser-induced damage threshold of preform materials was investigated in dependence on a varying thermal treatment and preparation procedure.Single and multi-pulse laser-induced damage thresholds of preforms (F300, Heraeus) were measured using a Q-switched Nd:YAG laser at 1064 nm wavelength emitting pulses with a duration of 15 ns, a pulse energy of 12 mJ and a repetition rate of 10 Hz. The temporal and spatial shape of the laser pulses were controlled accurately.Laser-induced damage thresholds in a range from 150 J cm⁻² to 350 J cm⁻² were determined depending on the number of pulses applied to the same spot, the thermal history and the polishing quality of the samples, respectively.     

Periodic surface structures on crystalline silicon created by 532 nm picosecond Nd:YAG laser pulses

Creation of laser-induced morphology features, particularly laser-induced periodic surface structures (LIPSS), by a 532 nm picosecond Nd:YAG laser on crystalline silicon is reported. The LIPSS, often termed ripples, were produced at average laser irradiation fluences of 0.7, 1.6, and 7.9 J cm⁻². Two types of ripples were registered: micro-ripples (at micrometer scale) in the form of straight parallel lines extending over the entire irradiated spot, and nano-ripples (at nanometer scale), apparently concentric, registered only at the rim of the spot, with the periodicity dependent on laser fluence. There are indications that the parallel ripples are a consequence of the partial periodicity contained in the diffraction modulated laser beam, and the nano-ripples are very likely frozen capillary waves. The damage threshold fluence was estimated at 0.6 J cm⁻².     

XPS study of silicon surface after ultra-low-energy ion implantation

Ultra-low-energy ion implantation of silicon with a hydrogen-terminated (0 0 1) surface was carried out using a mass-separated ³¹P⁺ ion beam. The ion energy was 30 eV, the displacement energy of silicon, and the ion doses were 6 × 10¹³ ions/cm². Annealing after the implantation was not carried out. The effects of ion implantation on the surface electrical state of silicon were investigated using X-ray photoelectron spectroscopy (XPS). The Si 2p peak position using XPS depends on the doping conditions because the Fermi level of the hydrogen-terminated silicon surface is unpinned. The Si 2p peak position of the specimen after ion implantation at a vacuum pressure of 3 × 10⁻⁷ Pa was shifted to the higher energy region. It suggested the possibility of phosphorus doping in silicon without annealing. In the case of ion implantation at 5 × 10⁻⁵ Pa, the Si 2p peak position was not shifted, and the peak was broadened because of the damage by the fast neutrals. Ultra-low-energy ion doping can be achieved at ultra-high-vacuum conditions.     

Picosecond laser ablation of nano-sized WTi thin film

Interaction of an Nd:YAG laser, operating at 532 nm wavelength and pulse duration of 40 ps, with tungsten-titanium (WTi) thin film (thickness, 190 nm) deposited on single silicon (100) substrate was studied. Laser fluences of 10.5 and 13.4 J/cm² were found to be sufficient for modification of the WTi/silicon target system. The energy absorbed from the Nd:YAG laser beam is partially converted to thermal energy, which generates a series of effects, such as melting, vaporization of the molten material, shock waves, etc. The following WTi/silicon surface morphological changes were observed: (i) ablation of the thin film during the first laser pulse. The boundary of damage area was relatively sharp after action of one pulse whereas it was quite diffuse after irradiation with more than 10 pulses; (ii) appearance of some nano-structures (e.g., nano-ripples) in the irradiated region; (iii) appearance of the micro-cracking. The process of the laser interaction with WTi/silicon target was accompanied by formation of plasma.     

The influence of the number of pulses on the morphological and photoluminescence properties of SrAl2O4:Eu,Dy thin films prepared by pulsed laser deposition

The current work reports on the influence of the number of laser pulses on the morphological and photoluminescence properties of SrAl₂O₄:Eu²⁺,Dy³⁺ thin films prepared by the pulsed laser deposition (PLD) technique. Atomic force microscopy (AFM) was used to study the surface topography and morphology of the films. The AFM data showed that the film deposited using a higher number of laser pulses was packed with a uniform layer of coarse grains. In addition, the surface of this film was shown to be relatively rougher than the films deposited at a lower number of pulses. Photoluminescence (PL) data were collected using the Cary Eclipse fluorescence spectrophotometer equipped with a monochromatic xenon lamp. An intense green photoluminescence was observed at 517 nm from the films prepared using a higher number of laser pulses. Consistent with the PL data, the decay time of the film deposited using a higher number of pulses was characteristically longer than those of the other films. The effects of laser pulses on morphology, topography and photoluminescence intensity of the SrAl₂O₄:Eu²⁺,Dy³⁺ thin films are discussed.     

Periodic surface nanostructures on polycrystalline ZnO induced by femtosecond laser pulses

Periodic surface nanostructures induced by femtosecond laser pulses on polycrystalline ZnO are presented. By translating the sample line-by-line under appropriate irradiation conditions, grating-like nanostructures with an average period of 160 nm are fabricated. The dependence of surface morphologies on the processing parameters, such as laser fluence, pulse number and laser polarization, are studied by scanning electronic microscope (SEM). In addition, photoluminescence (PL) analysis at room-temperature indicates that the PL intensity of the irradiated area increases significantly compared with the un-irradiated area. Using femtosecond laser pulses irradiation to fabricate periodic surface nanostructures on polycrystalline ZnO is efficient, simple and low cost, which shows great potential applications in ZnO-based optoelectronic devices.     

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.