Mg-based photocathodes prepared by ns, ps and fs PLD for the production of high brightness electron beams

Mg-based films have been prepared by pulsed laser deposition technique for photocathode applications. We have investigated the influence of pulse laser duration on morphology and photoemissive properties. Two laser sources have been used, generating pulses of 30 ns at 308 nm (XeCl excimer laser), 5 ps and 500 fs at 248 nm (KrF excimer laser) to grow Mg films onto Si and Cu substrates in high vacuum (∼10⁻⁷ Pa) and at room temperature. Morphological investigations carried out by scanning electron microscopy (SEM) have revealed that, in our experimental conditions, the number and the mean size of the droplets on the films surfaces decreases as the pulse laser duration shortens. The contamination level of Mg film surfaces have been studied by energy dispersive X-ray spectroscopy (EDX). The photoelectron performances in terms of quantum efficiency (QE) and emission stability have been tested in a UHV DC photodiode cell (10⁻⁷ Pa). Measures of the QE of the samples surfaces have revealed a decrease on the initial value for Mg-based photocathodes prepared by fs laser (from 7.8 × 10⁻⁴ to 6.6 × 10⁻⁴) PLD with respect to ps (from 6.2 × 10⁻⁴ to 7.4 × 10⁻⁴) and ns lasers (from 5.0 × 10⁻⁴ to 1.6 × 10⁻³). A comparison among Mg-based photocathodes prepared by ns, ps and fs PLD for the production of high brightness electron beams has been presented and discussed.     

Pulsed laser deposition of nanostructured Ag films

Ultra-thin (0.5-5 nm) films of Ag have been prepared by pulsed laser deposition in vacuum using a 26 ns KrF excimer laser at 1 J cm⁻². The deposition was controlled using a Langmuir ion probe and a quartz crystal thickness monitor. Transmission electron microscopy showed that the films are not continuous, but are structured on nanometer size scales. Optical absorption spectra showed the expected surface plasmon resonance feature, which shifted to longer wavelength and increased in strength as the equivalent film thickness was increased. It is shown that Maxwell Garnett effective medium theory can be used to calculate the main features of optical absorption spectra.     

Laser energy density, structure and properties of pulsed-laser deposited zinc oxide films

Zinc oxide thin films were deposited on soda lime glass substrates by pulsed laser deposition in an oxygen-reactive atmosphere at 20 Pa and a constant substrate temperature at 300 °C. A pulsed KrF excimer laser, operated at 248 nm with pulse duration 10 ns, was used to ablate the ceramic zinc oxide target. The structure, the optical and electrical properties of the as-deposited films were studied in dependence of the laser energy density in the 1.2-2.8 J/cm² range, with the aid of X-ray Diffraction, Atomic Force Microscope, Transmission Spectroscopy techniques, and the Van der Pauw method, respectively. The results indicated that the structural and optical properties of the zinc oxide films were improved by increasing the laser energy density of the ablating laser. The surface roughness of the zinc oxide film increased with the decrease of laser energy density and both the optical bang gap and the electrical resistivity of the film were significantly affected by the laser energy density.     

Study of temperature dependence and angular distribution of poly(9,9-dioctylfluorene) polymer films deposited by matrix-assisted pulsed laser evaporation (MAPLE)

Poly(9,9-dioctylfluorene) (PFO) polymer films were deposited by matrix-assisted pulsed laser evaporation (MAPLE) technique. The polymer was diluted (0.5 wt%) in tetrahydrofuran and, once cooled to liquid nitrogen temperature, it was irradiated with a KrF excimer laser. 10,000 laser pulses were used to deposit PFO films on 〈1 0 0〉 Si substrates at different temperatures (−16, 30, 50 and 70 °C). One PFO film was deposited with 16,000 laser pulses at a substrate temperature of 50 °C. The morphology, optical and structural properties of the films were investigated by SEM, AFM, PL and FTIR spectroscopy. SEM inspection showed different characteristic features on the film surface, like deflated balloons, droplets and entangled polymer filaments. The roughness of the films was, at least partially, controlled by substrate heating, which however had the effect to reduce the deposition rate. The increase of the laser pulse number modified the target composition and increased the surface roughness. The angular distribution of the material ejected from the target confirmed the forward ejection of the target material. PFO films presented negligible modification of the chemical structure respect to the bulk material.     

Opto-electrical properties of Ti-doped In2O3 thin films grown by pulsed laser deposition

By ablating titanium containing In₂O₃ target with a KrF excimer laser, highly conducting and transparent films on quartz were obtained to investigate the effects of growth temperature and oxygen pressure on the structural, optical and electrical properties of these films. We find that the transparency of the films depends more on the growth temperature and less on the oxygen pressure. Electrical properties, however, are found to be sensitive to both the growth temperature and oxygen pressure. We report in this paper that a growth temperature of 500 °C and an oxygen pressure of 7.5 × 10⁻⁷ bar lead to titanium-doped indium oxide films which have high mobility (up to 199 cm² V⁻¹ s⁻¹), low resistivity (9.8 × 10⁻⁵ Ω cm), and relatively high transmittance (∼88%).     

Influence of oxygen partial pressure on optoelectrical properties of aluminum-doped CdO thin films

Highly conducting and transparent aluminum-doped CdO thin films were deposited on quartz by ablating the sintered target of CdO containing 2 wt% of aluminum with a KrF excimer laser (λ = 248 nm and pulsed duration of 20 ns). The effect of oxygen partial pressure on structural, electrical, and optical properties was studied. It is observed that the (2 0 0) plane is highly preferred for the films grown under high oxygen pressure. The conductivity, carrier concentration and mobility of the films decrease with increase in the oxygen pressure after attaining maximum. Low resistivity (2.27 × 10⁻⁵ Ω cm), and high mobility (79 cm² V⁻¹ s⁻¹) is observed for the film grown under oxygen pressure of 1.0 × 10⁻³ mbar. The optical band gap is found varying between 2.68 and 2.90 eV for various oxygen pressure.     

On determining the spot size for laser fluence measurements

Energy fluence, defined as pulse energy over irradiated area, is a key parameter of pulsed laser processing. Nevertheless, most of the authors using this term routinely do not realize the problems related to the accurate measurement of the spot size. In the present paper we are aiming to approach this problem by ablating crystalline Si wafers with pulses of a commercial KrF excimer laser (λ = 248 nm, τ = 15 ns) both in vacuum and at ambient atmosphere. For any pulse energy, the size of the ablated area monotonously increases with increasing number of pulses. The difference in the ablated area could be as high as a factor of three when 2000 consecutive pulses impinge on the surface. The existence and extent of the gradual lowering of multi-pulse ablation threshold queries the applicability of routinely used procedure of dividing the pulse energy with the size of the ablated area exposed into either carbon-paper or a piece of Si with one or a few pulses when determining the fluence. A more quantitative way is proposed allowing comparison of results originating from different laboratories.     

Femtosecond pulsed laser deposition of diamond-like carbon films: The effect of double laser pulses

The bonding structure of carbon films prepared by pulsed laser deposition is determined by the plasma properties especially the change of the kinetic energy. Using double laser pulses the ablation process and the characteristics of the generated plasma can be controlled by the setting of the delay between the pulses. In our experiments, amorphous carbon films have been deposited in vacuum onto Si substrates by double pulses from a Ti:sapphire laser (180 fs, λ = 800 nm, at 1 kHz) and a KrF laser system (500 fs, λ = 248 nm, at 5 Hz). The intensities have been varied in the range of 3.4 × 10¹² to 2 × 10¹³ W/cm². The morphology and the main properties of the thin layers were investigated as a function of the time delay between the two ablating pulses (0-116.8 ps) and as a function of the irradiated area on the target surface. Atomic force microscopy, spectroscopic ellipsometry and Raman-spectroscopy were used to characterize the films. It was demonstrated that the change of the delay and the spot size results in the modification of the thickness distribution of the layers, and the carbon sp²/sp³ bonding ratio.     

Femtosecond laser ablation of silver foil with single and double pulses

The average ablation depth per pulse of silver foil by 130 fs laser pulses has been measured in vacuum over a range of three orders of magnitude of pulse fluence up to 900 J cm⁻². In addition, double pulses with separations up to 3.4 ns have been used to probe time scales of relevance for femtosecond ablation. The double pulse ablation depth, when each pulse fluence is 0.7 J cm⁻², falls to that of a single pulse as the pulse separation is increased from 0 ps to 700 ps. This time scale decreases to only 4 ps as the fluence is increased to 11 J cm⁻². It then jumps to 500 ps across a transition fluence where the slope of the ablation depth versus logarithmic fluence characteristic changes abruptly to a higher value. In addition, for pulse separations near 1000 ps, the second pulse can cause re-deposition of ejecta from the first pulse resulting in a double pulse ablation depth only 40% that of the first pulse alone. This has important implications for the interpretation of double pulse femto-LIBS intensities. Our results suggest that the optical properties of nano or mesoparticles play a significant role in double pulse ablation with large pulse separations.     

Matrix assisted pulsed laser evaporation of cinnamate-pullulan and tosylate-pullulan polysaccharide derivative thin films for pharmaceutical applications

We have demonstrated the successful thin film growth of two pullulan derivatives (cinnamate-pullulan and tosylate-pullulan) using matrix assisted pulsed laser evaporation (MAPLE). Our MAPLE system consisted of a KrF* laser, a vacuum chamber, and a rotating target holder cooled with liquid nitrogen. Fused silica and silicon (1 1 1) wafers were used as substrates. The MAPLE-deposited thin films were characterized by transmission spectrometry, profilometry, atomic force microscopy (AFM), Fourier transform infrared (FTIR) spectroscopy and Raman spectroscopy. The deposited layers ranged from 250 nm to 16.5 μm in thickness, depending on the laser fluence (0.065-0.5 J cm⁻²) and number of pulses applied for the deposition of one structure (1500-13,300). Our results confirmed that MAPLE was well-suited for the transfer of cinnamate-pullulan and tosylate-pullulan.     

Influence of the laser wavelength on the epitaxial growth and electrical properties of La0.8Sr0.2MnO3 films grown by excimer laser-assisted MOD

Epitaxial La_1−xSr_xMnO₃ (LSMO) films were prepared by excimer laser-assisted metal organic deposition (ELAMOD) at a low temperature using ArF, KrF, and XeCl excimer lasers. Cross-section transmission electron microscopy (XTEM) observations confirmed the epitaxial growth and homogeneity of the LSMO film on a SrTiO₃ (STO) substrate, which was prepared using ArF, KrF, and XeCl excimer lasers. It was found that uniform epitaxial films could be grown at 500 °C by laser irradiation. When an XeCl laser was used, an epitaxial film was formed on the STO substrate at a fluence range from 80 to 140 mJ/cm² of the laser fluence for the epitaxial growth of LSMO film on STO substrate was changed. When the LaAlO₃ (LAO) substrate was used, an epitaxial film was only obtained by ArF laser irradiation, and no epitaxial film was obtained using the KrF and XeCl lasers. When the back of the amorphous LSMO film on an LAO substrate was irradiated using a KrF laser, no epitaxial film formed. Based on the effect of the wavelength and substrate material on the epitaxial growth, formation of the epitaxial film would be found to be photo thermal reaction and photochemical reaction. The maximum temperature coefficient of resistance (TCR) of the epitaxial La_0.8Sr_0.2MnO₃ film on an STO substrate grown using an XeCl laser is 4.0%/K at 275 K. XeCl lasers that deliver stabilized pulse energies can be used to prepare LSMO films with good a TCR.     

Pulsed laser deposition of polyhydroxybutyrate biodegradable polymer thin films using ArF excimer laser

We demonstrated the pulsed laser deposition (PLD) of high quality films of a biodegradable polymer, the polyhydroxybutyrate (PHB). Thin films of PHB were deposited on KBr substrates and fused silica plates using an ArF (λ = 193 nm, FWHM = 30 ns) excimer laser with fluences between 0.05 and 1.5 J cm⁻². FTIR spectroscopic measurements proved that at the appropriate fluence (0.05, 0.09 and 0.12 J cm⁻²), the films exhibited similar functional groups with no significant laser-produced modifications present. Optical microscopic images showed that the layers were contiguous with embedded micrometer-sized grains. Ellipsometric results determined the wavelength dependence (λ ∼ 245-1000 nm) of the refractive index and absorption coefficient which were new information about the material and were not published in the scientific literature. We believe that our deposited PHB thin films would have more possible applications. For example to our supposal the thin layers would be applicable in laser induced forward transfer (LIFT) of biological materials using them as absorbing thin films.     

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.     

Pulsed-laser crystallization and epitaxial growth of metal-organic films of Ca-doped LaMnO3 on STO and LSAT substrates

Ca-doped LaMnO₃ (LCMO) thin films have been successfully prepared on SrTiO₃ (STO) and [(LaAlO₃)_0.3-(SrAlTaO₆)_0.7] (LSAT) substrates using the excimer laser assisted metal-organic deposition (ELAMOD) process. The crystallization and the epitaxial growth of the amorphous metal-organic LCMO thin films have been achieved using a KrF excimer laser irradiation while the substrates were kept at constant temperature of 500 °C. Epitaxial films were obtained using laser fluence in the interval of 50-120 mJ/cm². The microstructure of the LCMO films was studied using cross-section transmission electron microscopy. High quality of LCMO films having smooth surfaces and sharp interfaces were obtained on both the STO and the LSAT substrates. The effect of the laser fluence on the temperature coefficient of resistance (TCR) was investigated. The largest values of TCR of the LCMO grown on the LSAT and the STO substrates of 8.3% K⁻¹ and 7.46% K⁻¹ were obtained at different laser fluence of 80 mJ/cm² and 70 mJ/cm², respectively.     

Deposition of aluminum nitride thin film on Si(1 1 1) by KrF excimer laser and its characterizations

We present the deposition of aluminum nitride (AlN) thin film by KrF excimer laser sputtering and the study of the effects of substrate temperature and laser fluences. Deposition rate of AlN thin film at 0.3 Å/pulse has been achieved with laser fluence of 1500 mJ/cm² and at substrate temperature of 250 K, and this shows the enhancement of the deposition rate at low substrate temperature. Surface morphology of the deposited films is characterized by atomic force microscopy (AFM). In addition, the electrical performance of the MIS devices with AlN thin films prepared in this experiment has been characterized.     

High level compressive residual stresses produced in aluminum alloys by laser shock processing

Laser shock processing (LSP) has been proposed as a competitive alternative technology to classical treatments for improving fatigue and wear resistance of metals. We present a configuration and results for metal surface treatments in underwater laser irradiation at 1064 nm. A convergent lens is used to deliver 1.2 J/cm² in a 8 ns laser FWHM pulse produced by 10 Hz Q-switched Nd:YAG, two laser spot diameters were used: 0.8 and 1.5 mm.Results using pulse densities of 2500 pulses/cm² in 6061-T6 aluminum samples and 5000 pulses/cm² in 2024 aluminum samples are presented. High level of compressive residual stresses are produced −1600 MPa for 6061-T6 Al alloy, and −1400 MPa for 2024 Al alloy. It has been shown that surface residual stress level is higher than that achieved by conventional shot peening and with greater depths. This method can be applied to surface treatment of final metal products.     

Structural characterization of AlN films synthesized by pulsed laser deposition

We obtained AlN thin films by pulsed laser deposition (PLD) from a polycrystalline AlN target using a pulsed KrF* excimer laser source (248 nm, 25 ns, intensity of ∼4 × 10⁸ W/cm², repetition rate 3 Hz, 10 J/cm² laser fluence). The target-Si substrate distance was 5 cm. Films were grown either in vacuum (10⁻⁴ Pa residual pressure) or in nitrogen at a dynamic pressure of 0.1 and 10 Pa, using a total of 20,000 subsequent pulses. The films structure was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and spectral ellipsometry (SE). Our TEM and XRD studies showed a strong dependence of the film structure on the nitrogen content in the ambient gas. The films deposited in vacuum exhibited a high quality polycrystalline structure with a hexagonal phase. The crystallite growth proceeds along the c-axis, perpendicular to the substrate surface, resulting in a columnar and strongly textured structure. The films grown at low nitrogen pressure (0.1 Pa) were amorphous as seen by TEM and XRD, but SE data analysis revealed ∼1.7 vol.% crystallites embedded in the amorphous AlN matrix. Increasing the nitrogen pressure to 10 Pa promotes the formation of cubic (≤10 nm) crystallites as seen by TEM but their density was still low to be detected by XRD. SE data analysis confirmed the results obtained from the TEM and XRD observations.     

Chemical composition of ZrC thin films grown by pulsed laser deposition

ZrC films were grown on (1 0 0) Si substrates by the pulsed laser deposition (PLD) technique using a KrF excimer laser working at 40 Hz. The nominal substrate temperature during depositions was set at 300 °C and the cooling rate was 5 °C/min. X-ray diffraction investigations showed that films deposited under residual vacuum or under 2 × 10⁻³ Pa of CH₄ atmosphere were crystalline, exhibiting a (2 0 0)-axis texture, while those deposited under 2 × 10⁻² Pa of CH₄ atmosphere were found to be equiaxed and with smaller grain size. The surface elemental composition of as-deposited films, analyzed by Auger electron spectroscopy (AES) and X-ray photoelectron spectroscopy (XPS), showed the usual high oxygen contamination of carbides. Once the topmost 2-4 nm region was removed, the oxygen concentration rapidly decreased, down to around 3-8% only in bulk. Simulations of the X-ray reflectivity (XRR) curves indicated a smooth surface morphology, with roughness values below 1 nm (rms) and films density values of around 6.30-6.45 g/cm³, very close to the bulk density. The growth rate, estimated from thickness measurements by XRR was around 8.25 nm/min. Nanoindentation results showed for the best quality ZrC films a hardness of 27.6 GPa and a reduced modulus of 228 GPa.     

Reactive pulsed laser deposition of gold nitride thin films

We report on the growth and characterization of gold nitride thin films on Si 〈1 0 0〉 substrates at room temperature by reactive pulsed laser ablation. A pure (99.95%) Au target was ablated with KrF excimer laser pulses in nitrogen containing atmosphere (N₂ or NH₃). The gas ambient pressure was varied in the range 0.1-100 Pa. The morphology of the films was studied by using optical, scanning electron and atomic force microscopy, evidencing compact films with RMS roughness in the range 3.6-35.1 nm, depending on the deposition pressure. Rutherford backscattering spectrometry and energy dispersion spectroscopy (EDS) were used to detect the nitrogen concentration into the films. The EDS nitrogen peak does not decrease in intensity after 2 h annealing at 250 °C. Film resistivity was measured using a four-point probe and resulted in the (4-20) × 10⁻⁸ Ω m range, depending on the ambient pressure, to be compared with the value 2.6 × 10⁻⁸ Ω m of a pure gold film. Indentation and scratch measurements gave microhardness values of 2-3 GPa and the Young's modulus close to 100 GPa. X-ray photoemission spectra clearly showed the N 1s peak around 400 eV and displaced with respect to N₂ phase. All these measurements point to the formation of the gold nitride phase.     

Femtosecond laser-induced damage of gold films

Single- and multi-shot ablation thresholds of gold films in the thickness range of 31-1400 nm were determined employing a Ti:sapphire laser delivering pulses of 28 fs duration, 793 nm center wavelength at 1 kHz repetition rate. The gold layers were deposited on BK7 glass by an electron beam evaporation process and characterized by atomic force microscopy and ellipsometry. A linear dependence of the ablation threshold fluence F_th on the layer thickness d was found for d ≤ 180 nm. If a film thickness of about 180 nm was reached, the damage threshold remained constant at its bulk value. For different numbers of pulses per spot (N-on-1), bulk damage thresholds of ∼0.7 J cm⁻² (1-on-1), 0.5 J cm⁻² (10-on-1), 0.4 J cm⁻² (100-on-1), 0.25 J cm⁻² (1000-on-1), and 0.2 J cm⁻² (10000-on-1) were obtained experimentally indicating an incubation behavior. A characteristic layer thickness of L_c ≈ 180 nm can be defined which is a measure for the heat penetration depth within the electron gas before electron-phonon relaxation occurs. L_c is by more than an order of magnitude larger than the optical absorption length of α⁻¹ ≈ 12 nm at 793 nm wavelength.