Dynamics of femtosecond laser-produced plasma ions

We investigated the ion laser-produced plasma plume generated during ultrafast laser ablation of copper and silicon targets in high vacuum. The ablation plasma was induced by ≈50 fs, 800 nm Ti:Sa laser pulses irradiating the target surface at an angle of 45°. An ion probe was used to investigate the time-of-flight profiles of the emitted ions in a laser fluence range from the ablation threshold up to ≈10 J/cm². The angular distribution of the ion flux and average velocity of the produced ions were studied by moving the ion probe on a circle around the ablation spot. The angular distribution of the ion flux is well described by an adiabatic and isentropic model of expansion of a plume produced by laser ablation of solid targets. The angular distribution of the ion flux narrows as the laser pulse fluence increases. Moreover, the ion average velocity reaches values of several tens of km/s, evidencing the presence of ions with kinetic energy of several hundred eV. Finally, the ion flux energy is confined in a narrow angular region around the target normal.     

Laser irradiation effects on the surface,structural and mechanical properties of Al–Cu alloy 2024

Laser irradiation effects on surface, structural and mechanical properties of Al–Cu–Mg alloy (Al–Cu alloy 2024) have been investigated. The specimens were irradiated for various fluences ranging from 3.8 to 5.5 J/cm² using an Excimer (KrF) laser (248 nm, 18 ns, 30 Hz) under vacuum environment. The surface and structural modifications of the irradiated targets have been investigated by scanning electron microscope (SEM) and X-ray diffractometer (XRD), respectively. SEM analysis reveals the formation of micro-sized craters along the growth of periodic surface structures (ripples) at their peripheries. The size of the craters initially increases and then decreases by increasing the laser fluence. XRD analysis shows an anomalous trend in the peak intensity and crystallite size of the specimen irradiated for various fluences. A universal tensile testing machine and Vickers microhardness tester were employed in order to investigate the mechanical properties of the irradiated targets. The changes in yield strength, ultimate tensile strength and microhardness were found to be anomalous with increasing laser fluences. The changes in the surface and structural properties of Al–Cu alloy 2024 after laser irradiation have been associated with the changes in mechanical properties.     

Time-resolved and integrated angular distributions of plume ions from silver at low and medium laser fluence

Laser impact on metals in the UV regime results in a significant number of ablated plume ions even at moderate fluence (0.7–2.4 J/cm²). The ablated particles are largely neutrals at the lowest fluence, but the fraction of ions increases strongly with fluence. The ion flow in different directions from a silver target irradiated by a laser beam at a wavelength of 355 nm in vacuum was measured with a hemispherical array of Langmuir probes. The time-of-flight spectra in all directions, as well as the total angular yield were determined. The angular distribution peaks strongly in forward direction with increasing fluence and can be well approximated by Anisimov’s model. Typically, the spectra of silver ions peak from 70 eV up to 145 eV in a direction close to the normal of the target surface with increasing fluence. With increasing observation angle, the time-of-flight spectra exhibit a peak at longer flight times, i.e., at a lower kinetic energy. At the highest fluence, the ionized fraction of the ablated particles in the plume increases up to 0.5.     

Two-dimensional imaging of atomic and nanoparticle components in copper plasma plume produced by ultrafast laser ablation

We report on the spatial and temporal evolution of the plume generated during ultrafast laser ablation of a pure copper target with 800 nm, ≈50 fs, Ti: Sapphire laser pulses. Time-gated imaging was used to record 2-dimensional images of plume populations. The temporal evolution of neutral (Cu*), and ionic (Cu⁺) components of the plume are separately imaged by exploiting bandpass interference filters, while nanoparticles are investigated by collecting their characteristic broadband emission. The ionic component of the plume moves two to three times faster than the neutral component, with a velocity which is almost independent of laser fluence. Plume emission intensity variations at different fluences and delay times are studied for both atomic and nanoparticle components.     

Non-equilibrium plasma production by pulsed laser ablation of gold

A gold target has been irradiated with a Q-switched Nd:Yag laser having 1064?nm wavelength, 9?ns pulse width, 900?mJ maximum pulse energy and a maximum power density of the order of 10¹⁰?W/cm². The laser–target interaction produces a strong gold etching with production of a plasma in front of the target. The plasma contains neutrals and ions having a high charge state. Time-of-flight (TOF) measurements are presented for the analysis of the ion production and ion velocity. A cylindrical electrostatic deflection ion analyzer permits measurement of the yield of the emitted ions, their charge state and their ion energy distribution. Measurements indicate that the ion charge state reaches 6⁺ and 10⁺ at a laser fluence of 100?J/cm² and 160?J/cm², respectively. The maximum ion energy reaches about 2?keV and 8?keV at these low and high laser fluences, respectively. Experimental ion energy distributions are given as a function of the ion charge state. Obtained results indicate that electrical fields, produced in the plume, along the normal to the plane of the target surface, exist in the unstable plasma. The electrical fields induce ion acceleration away from the target with a final velocity dependent on the ion charge state. The ion velocity distributions follow a “shifted Maxwellian distribution”, which the authors have corrected for the Coulomb interactions occurring inside the plasma.     

Effect of 100 MeV O7+ ion beam irradiation on structural,optical and electronic properties of SnO2 thin films

In this paper, we present the impact of swift heavy ion beam irradiation on the structural, optical and electronic properties of SnO₂ thin films. Thin films were deposited using the pulsed laser deposition technique on Al₂O₃ substrates. Atomic force microscopy, X-ray diffraction, UV–visible absorption and temperature-dependent resistivity measurements were performed to explore the morphological, structural, optical and electronic properties of the as-deposited and irradiated samples. The peak intensity of the (200) peak was found to decrease monotonously with increasing irradiation fluence. The band gap energy of the 1×10¹¹ ion/cm² irradiated sample was found to increase. The electrical resistivity of the samples showed a continuous increase with the irradiation fluence.     

Biocompatible film deposition by using Nd:YAG pulsed laser

A Nd:YAG laser operating at the fundamental wavelength (1064 nm) and at the second harmonic (532 nm), with 9 ns pulse duration, 100–900 mJ pulse energy, and 30 Hz repetition rate mode, was employed to ablate in vacuum (10^?6 mbar) biomaterial targets and to deposit thin films on substrate backings. Titanium target was ablated at the fundamental frequency and deposited on near-Si substrates. The ablation yield increases with the laser fluence and at 40 J/cm ² the ablation yield for titanium is 1.2×10¹⁶ atoms/pulse. Thin film of titanium was deposited on silicon substrates placed at different distance and angles with respect to the target and analysed with different surface techniques (optical microscopy, scanning electron spectrosopy (SEM), and surface profile).

Hydroxyapatite (HA) target was ablated to the second harmonic and thin films were deposited on Ti and Si substrates. The ablation yield at a laser fluence of 10 J/cm ² is about 5×10¹⁴ HA molecules/pulse. Thin film of HA, deposited on silicon substrates placed at different distance and angles with respect to the target, was analysed with different surface techniques (optical microscopy, SEM, and Raman spectroscopy).

Metallic films show high uniformity and absence of grains, whereas the bio-ceramic film shows a large grain size distribution. Both films found special application in the field of biomaterial coverage.     

Surface topography of ultrashort laser-irradiated CaF2

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

Study of 2<Emphasis Type="Italic">ω</Emphasis> and 3/2<Emphasis Type="Italic">ω</Emphasis> harmonics in ultrashort high-intensity laser plasma interaction

An experimental study is presented on measurements of optical spectrum of the laser light scattered from solid surface irradiated by Ti:sapphire laser pulses up to an intensity of 1.2 × 10¹⁸ W cm⁻². The spectrum has well-defined peaks at wavelengths corresponding to 2ω and 3/2ω radiations. The spectral features vary with the laser intensity and show blue-shift with increasing laser intensity. At a constant laser fluence, the spectrum is red-shifted with increasing laser pulse duration. The observed results are explained in terms of the density scale length variation of the plasma and laser chirp.     

Production of nanostructures on bulk metal samples by laser ablation for fabrication of low-reflective surfaces

Nanostructure formation on bulk noble metals (copper, gold and silver) by a femtosecond laser was studied aiming at the production of low-reflectivity surfaces. The target surface was irradiated with the beam of a 775 nm wavelength and 150 fs pulse duration Ti:sapphire laser. The fluence was in the 16–2000 mJ/cm² range, while the average pulse number was varied between 10 and 1000 depending on the scanning speed of the sample stage. The reflectivity of the treated surfaces was measured with a visible–near-infrared microspectrometer in the 450–800 nm range, while the morphology was studied with a scanning electron microscope. A strong correlation was found between the decreasing reflectivity and the nanostructure formation on the irradiated surface; however, the morphology of silver significantly differed from those of copper and gold. For the two latter metals a dense coral-like structure was found probably as a result of cluster condensation in the ablation plume followed by diffusion-limited aggregation. In the case of silver the surface was covered by nanodroplets, which formation was probably influenced by the ‘spitting’ caused by ambient oxygen absorption in the molten silver followed by its fast release during the resolidification.     

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.     

Production of ion and electron streams by pulsed-laser ablation of Ta and Cu

A Nd:YAG laser with 10⁹ W/cm ² pulse intensity, operating at 532 nm wavelength, is used to ablate Ta and Cu targets placed in vacuum. The ablation process generates a plasma in front of the target surface, which expands along the normal to target surface. The ion and electron emissions from the plasma were measured by Faraday cups placed at different angles with respect to the normal to target surface. In the range of laser intensities from 10⁷ to 10⁹ W/cm², the fast electron yield is lower than the ion yield and it increases at higher laser intensities. The ablation threshold, the emission yield, the ion and electron average energies and the plasma ion and electron temperatures were measured for ion and fast electron streams.     

Reflection of high-intensity nanosecond Nd:YAG laser pulses by metals

Total reflectivity of silver and molybdenum samples irradiated by high-intensity nanosecond Nd:YAG laser pulses in air of atmospheric pressure is experimentally studied as a function of laser fluence in the range of 0.1–100 J/cm². The study shows that at laser fluences below the plasma formation threshold the total reflectivity of both silver and molybdenum remains virtually equal to the table room-temperature reflectivity values. The total reflectivity of these metals begins to decrease at a laser fluence of the plasma formation threshold. As the laser fluence increases above the plasma formation threshold, the reflectivity sharply drops to a low value and then remains unchanged with further increasing laser fluence. Calculation of the surface temperature at the plasma formation threshold fluence shows that the surface temperature value is substantially below the melting point that indicates an important role of the surface nanostructural defects in the plasma formation on a real sample due to their enhanced heating caused by both plasmonic absorption and plasmonic nanofocusing.     

Non-equilibrium plasma production by pulsed laser ablation of gold

A gold target has been irradiated with a Q-switched Nd:Yag laser having 1064\,\hbox{nm} wavelength, 9\,\hbox{ns} pulse width, 900\,\hbox{mJ} maximum pulse energy and a maximum power density of the order of 10^{10}\,\hbox{W}/\hbox{cm}^2 . The laser-target interaction produces a strong gold etching with a production of a plasma in front of the target. The plasma contains neutrals and ions having high charge state. Time-of-flight measurements are presented for the analysis of the ion production and ion velocity. A cylindrical electrostatic deflection ion analyzer permits to measure the yield of the emitted ions, their charge state and their ion energy distribution. Measurements indicate that the ion charge state reaches 6^+ and 10^+ at a laser fluence of 100\,\rm{J/cm}^2 and 160\,\rm{J/cm}^2 , respectively. The maximum ion energy reaches about 2\,\hbox{keV} and 8\,\hbox{keV} at these low and at high laser fluence, respectively. Experimental ion energy distributions are given as a function of the ion charge state. Obtained results indicate that electrical fields, produced in the plume, along the normal to the plane of the target surface, exist in the unstable plasma. The electrical fields induce ion acceleration away from the target with a final velocity dependent on the ion charge state. The ion velocity distributions follow a "shifted Maxwellian distribution", which the authors have corrected for the Coulomb interactions occurring inside the plasma.     

Surface and Bulk Structure Characterization of Proton (3 MeV) Irradiated Polycarbonate

Polycarbonate (Makrofol‐N) thin films were irradiated with protons (3 MeV) under vacuum at room temperature with the fluence ranging from 1×10¹⁴ to 1×10¹⁵ protons cm^?2. The change in surface morphology, optical properties, degradation of the functional groups, and crystallinity of the proton‐irradiated polymers were investigated with atomic force microscopy (AFM), UV‐VIS, and Fourier‐transform infrared (FTIR) spectroscopy, and X‐ray diffraction (XRD) techniques, respectively. AFM shows that the root mean square (RMS) roughness of the irradiated polycarbonate surface increases with the increment of ion fluence. The UV‐VIS analysis revealed that in Makrofol‐N the optical band gap decreased by 30% at highest fluence of 1×10¹⁵ protons cm^?2. The band gap can be correlated to the number of carbon atoms, M, in a cluster with a modified Robertson's equation. The cluster size in the proton‐irradiated Makrofol‐N increased from 112 to 129 atoms with the increase of fluence from 1×10¹⁴ to 1×10¹⁵ protons cm^?2. FTIR spectra of proton (3 MeV) irradiated Makrofol‐N showed a strong decrease of almost all absorption bands at about 1× 10¹⁴ protons cm^?2. However, beyond a higher critical dose an increase in intensity of almost all characteristic bands was noticed. The appearance of a new peak at 3,500 cm^?1 (‐OH groups) was observed at the higher fluences in the FTIR spectra of proton‐irradiated polycarbonate. XRD measurements showed an increase of full width at half maximum (FWHM) and the average intermolecular spacing of the main peak, which may be due to the increase of chain scission and the introduction of ‐OH groups in the proton irradiated polycarbonate.     

Features of plasma plume evolution and material removal efficiency during femtosecond laser ablation of nickel in high vacuum

We present an experimental characterization describing the characteristics features of the plasma plume dynamics and material removal efficiency during ultrashort, visible (527 nm, ≈300 fs) laser ablation of nickel in high vacuum. The spatio-temporal structure and expansion dynamics of the laser ablation plasma plume are investigated by using both time-gated fast imaging and optical emission spectroscopy. The spatio-temporal evolution of the ablation plume exhibits a layered structure which changes with the laser pulse fluence F. At low laser fluences (F<0.5 J/cm²) the plume consists of two main populations: fast Ni atoms and slower Ni nanoparticles, with average velocities of ≈10⁴ m/s for the atomic state and ≈10² m/s for the condensed state. At larger fluences (F>0.5 J/cm²), a third component of much faster atoms is observed to precede the main atomic plume component. These atoms can be ascribed to the recombination of faster ions with electrons in the early stages of the plume evolution. A particularly interesting feature of our analysis is that the study of the ablation efficiency as a function of the laser fluence indicates the existence of an optimal fluence range (a maximum) for nanoparticles generation, and an increase of atomization at larger fluences. PACS 52.50.-b; 52.38.Mf; 79.20.Ds; 81.07.-b     

Material ablation and plasma plume expansion study from Fe and graphite targets in Ar gas atmosphere

Study of expansion dynamics of pulsed-laser ablation plasmas from Fe and graphite targets is presented. A 532 nm Q-switched Nd:YAG laser with fluence of 30 J cm⁻² is used to ablate the Fe and graphite targets in various Ar ambient gas pressures. Plasma ablation parameters for the two target materials are estimated using snow-plow and shock-wave models, which show that the laser beam energy deposited to ablated species remains at 70% for both targets at all ambient pressures. The plume splitting was observed, more prominently, for Fe plasma as it moves faster compared to graphite plasma. The difference in plasma plume fronts’ speeds for different targets was attributed to the significant difference in mass of the ablated plasma for two targets, as estimated from simulation results.     

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.     

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.      

Effects of phase explosion in pulsed laser deposition of nickel thin film and sub-micron droplets

Nickel (Ni) thin films were deposited on glass substrates in high vacuum and at room temperature with third-harmonic or 355-nm output from a nanosecond Nd:YAG laser. At low laser fluence of 1 J/cm², the deposition rate was about 0.0016 nm/shot which increased linearly until 4 J/cm². Above 4 J/cm², the onset of phase explosion in the ablation abruptly increased the optical emission intensity from laser-produced Ni plume as well as thin-film deposition rate by about 6×. The phase explosion also shifted the size distribution and number density of Ni droplets on its thin-film surface. On the other hand, the surface structures of the ablated Ni targets were compared between the scan-mode and the fixed-mode ablations, which may suggest that droplets observed on the thin-film surface were caused by direct laser-induced splashing of molten Ni rather than vapour-to-cluster condensation during the plume propagation.