Optical emission spectroscopy investigation of an ultra-short laser induced titanium plasma reheated by a ns laser pulse

The dynamics of a titanium plasma species, induced in air by coupling a fs-ablating laser pulse with an orthogonal ns-reheating laser source placed at the fixed distance of 1.0 mm from the target surface, has been followed by temporally resolved emission spectroscopy. The temporal evolutions of plasma features such as excitation temperatures and electron densities have been evaluated by using two different laser energies of the first fs-ablating laser pulse (0.8 mJ and 3.0 mJ). Optimum inter-pulse delay times, experimentally determined, of 250 μs and 500 μs were used for the fs laser energy of 3.0 mJ and 0.8 mJ, respectively. By experimental inspections of the main plasma species electronic transitions so obtained, a strong enhancement was evaluated up to one and two orders of magnitude for Ti(I) and Ti(II), respectively. Independently from the fs laser energy employed, the plasma features showed the same temporal behaviour implying that the ns-reheating characteristics of this process belong to the reheating mechanism itself. The experimental results have been discussed and the excited species evolutions and elementary processes involved, as well as, the local thermodynamic equilibrium departures, have been outlined.     

Recombination emissions and spectral blueshift of pump radiation from ultrafast laser induced plasma in a planar water microjet

We report spectroscopic investigations of an ultrafast laser induced plasma generated in a planar water microjet. Plasma recombination emissions along with the spectral blueshift and broadening of the pump laser pulse contribute to the total emission. The laser pulses are of 100 fs duration, and the incident intensity is around 10¹⁵ W/cm². The dominant mechanisms leading to plasma formation are optical tunnel ionization and collisional ionization. Spectrally resolved polarization measurements show that the high frequency region of the emission is unpolarized whereas the low frequency region is polarized. Results indicate that at lower input intensities the emission arises mainly from plasma recombinations, which is accompanied by a weak blueshift of the incident laser pulse. At higher input intensities strong recombination emissions are seen, along with a broadening and asymmetric spectral blueshift of the pump laser pulse. From the nature of the blueshifted laser pulse it is possible to deduce whether the rate of change of free electron density is a constant or variable within the pulse lifetime. Two input laser intensity regimes, in which collisional and tunnel ionizations are dominant respectively, have been thus identified.     

fs/ns dual-pulse LIBS analytic survey for copper-based alloys

The quantitative analytic capability of a fs/ns dual-pulse Laser-Induced Breakdown Spectroscopy technique, based on the orthogonal reheating of a fs-laser ablation plume by a ns-laser pulse, is presented. In this work, it is shown how the effect played by the delay times between the two laser beams can vary the analytical response of this dual-pulse LIBS configuration. In order to address this task, the Sn, Pb and Zn calibration curves of five certified copper-based samples have been investigated. These calibration curves have been obtained, in air at atmospheric pressure, by integrating the emission data collected in two different inter-pulse delay zones, one in the delay interval of 1-41 μs, the other within the range of 46-196 μs. For drawing the species calibration curves, the emission intensities of the considered Pb(I), Sn(I) and Zn(I) electronic transitions have been normalized with a non-resonant Cu(I) emission line. The experimental results have shown that, by varying the inter-pulse delay between the two laser beams, complementary analytical results can be induced. By considering at once all data acquired within the inter-pulse delay time of 1-196 μs, this hypothesis has been strengthened. The calibration curves obtained in this way are characterized by excellent linear regression coefficients (0.988-0.999) despite of the large Sn, Pb and Zn compositional variation of the targets employed. The results presented reveal, for the first time, that, by taking into account the role played by the inter-pulse delay time between the two laser beams, the fs/ns dual-pulse LIBS configuration here used can be improved and provide very good opportunities for performing quantitative analysis of copper-based alloys.     

Characterization of the laser ablation plasma used for the deposition of amorphous carbon

The plasma produced by laser ablation of a graphite target was studied by means of optical emission spectroscopy and a Langmuir planar probe. Laser ablation was performed using a Nd:YAG laser with emission at the fundamental line with pulse length of 28 ns. In this work, we report the behavior of the mean kinetic energy of plasma ions and the plasma density, as a function of the laser fluence (J/cm²), and the target to probe (substrate) distance. The characterized regimes were employed to deposit amorphous carbon at different values of kinetic energy of the ions and plasma density. The mean kinetic energy of the ions could be changed from 40 to 300 eV, and the plasma density could be varied from 1 × 10¹² to 7 × 10¹³ cm⁻³. The main emitting species were C⁺ (283.66, 290.6, 299.2 and 426.65 nm) and C⁺⁺ (406.89 and 418.66 nm) with the C⁺ (426.65 nm) being the most intense and that which persisted for the longest times. Different combinations of the plasma parameters yield amorphous carbon with different structures. Low levels (about 40 eV) of ion energy produce graphitic materials, while medium levels (about 200 eV) required the highest plasma densities in order to increase the CC sp³ bonding content and therefore the hardness of the films. The structure of the material was studied by means of Raman spectroscopy, and the hardness and elastic modulus by depth sensitive nanoindentation.     

Nanosecond pulse laser melting investigation by IR radiometry and reflection-based methods

Experimental system for nanosecond laser melting investigation was developed containing three independent noncontact methods: infrared radiometry, time-resolved reflectivity of He-Ne laser and sample surface reflected KrF heating laser pulse. The system was applied to the investigation of laser melting of Cu, Mo, Ni, Si, Sn, Ti, steel ?SN 15330 and stainless steel ?SN 17246 samples. For metallic samples the IR radiometry signal was transformed to temperature. Obtained surface temperature and reflectivity spectra in nanosecond time scale (10-1000 ns) for wide range of energy densities (100-5500 mJ cm⁻²) are presented. Interesting evolutions were found. Melting thresholds and melting durations were determined from the measured curves. The applicability of the methods is evaluated.     

Two-color laser desorption of nanostructured MgO thin films

Neutral magnesium atom emission from nanostructured MgO thin films is induced using two-color nanosecond laser excitation. We find that combined vis/UV excitation, for single-color pulse energies below the desorption threshold, induces neutral Mg-atom emission with hyperthermal kinetic energies in the range of 0.1-0.2 eV. The observed metal atom emission is consistent with a mechanism involving rapid electron transfer to three-coordinated Mg surface sites. The two-color Mg-atom signal is significant only for parallel laser polarizations and temporally overlapped laser pulses indicating that intermediate excited states are short-lived compared to the 5 ns laser pulse duration.     

Femtosecond laser-induced dynamic alignment in Coulomb explosion of CO: Roles of laser wavelength, intensity and pulse duration

Dependences of dynamic alignment of CO molecules induced by intense femtosecond laser fields on laser wavelength, intensity and pulse duration are investigated by numerical simulations. A counting approach and a fourth-order Runge-Kutta algorithm are used to calculate the angular distribution and the time evolution of molecules. A two-step Coulomb explosion model of diatomic molecules in intense laser fields is used to determine the instant that CO molecular dynamic alignment is over. Our calculating results show that the linear polarizability and the damping force play an important role in the angular rotation of CO molecule in conditions of 800 nm laser wavelength and 10¹⁵ W/cm² laser intensity. The contributions of the second-order field-induced dipole moment and the higher-order correction term to molecular rotation acceleration comparing to the linear polarizability and damping force are negligible. The extent of dynamic alignment of CO molecules reduces with the increasing of laser intensity. The dynamic alignment time of CO molecules is tightly connected to the laser pulse duration. The angular distributions of CO molecules as the laser pulse length varied from 50 to 250 fs at laser intensity of 3×10¹⁴ W/cm² are shown and discussed.     

Silicon donor and Stokes terahertz lasers

Two types of lasers based on hydrogen-like impurity-related transitions in bulk silicon operate at frequencies between 1 and 7 THz (wavelength range of 50-230 μm). These lasers operate under mid-infrared optical pumping of n-doped silicon crystals at low temperatures (<30 K). Dipole-allowed optical transitions between particular excited states of group-V substitutional donors are utilized in the first type of terahertz silicon lasers. These lasers have a gain ∼1-3 cm⁻¹ above the laser thresholds (>1 kW cm⁻²) and provide 10 ps-1 μs pulses with a few mW output power on discrete lines. Raman-type Stokes stimulated emission in the range 4.6-5.8 THz has been observed from silicon crystals doped by antimony and phosphorus donors when optically excited by radiation from a tunable infrared free electron laser. The scattering occurs on the 1s(E)→1s(A₁) donor electronic transition accompanied by an emission of the intervalley transverse acoustic g-phonon. The Stokes lasing has a peak power of a few tenths of a mW and a pulse width of a few ns. The Raman optical gain is about 7.4 cm GW⁻¹ and the optical threshold intensity is ∼100 kW cm⁻².     

Femtosecond laser ablation of crystals SiO2 and YAG

Damage threshold of crystals SiO₂ and YAG against 60-900 fs, 800 nm laser pulses are reported. The breakdown mechanisms were discussed based on the double-flux model and Keldysh theory. We found that impact ionization plays the important role in the femtosecond laser-induced damage in crystalline SiO₂, while the roles of photoionization and impact ionization in YAG crystals depend on the laser pulse durations.     

Simulation of THz emission from laser interaction with plasmas

One-dimensional particle-in-cell (PIC) program is used to simulate the generation of high power terahertz (THz) emission from the interaction of an ultrashort intense laser pulse with underdense plasma. The spectra of THz radiation are discussed under different laser intensity, pulse width, incident angle and density scale length. High-amplitude electron plasma wave driven by a laser wakefield can produce powerful THz emission through linear mode conversion under certain conditions. With incident laser intensity of 10¹⁸ W/cm², the generated emission is computed to be of the order of several MV/cm field and tens of MW level power. The corresponding energy conversion efficiency is several ten thousandths, which is higher then the efficiency of other THz source and suitable for the studies of THz nonlinear physics.     

Studies of craters’ dimension for long-pulse laser ablation of metal targets at various experimental conditions

Long pulse laser shots of the PALS iodine laser in Prague have been used to obtain metal target ablation at various experimental conditions. Attention is paid mainly to the dependencies of the crater diameter on the position of minimum laser-focus spot with regard to the target surface, by using different laser wavelengths and laser energies. Not only a single one, but two minima, independently of the wavelength, of the target irradiation angle and of the target material, were recorded. Significant asymmetries, ascribed to the non-linear effects of intense laser beam with pre-formed plasma, were found, too. Estimations of ejected mass per laser pulse are reported and used to calculate the efficiency of laser-driven loading. Results on metal target ablation and crater formation at high intensities (from 2 × 10¹³ to 3 × 10¹⁶ W/cm²) are presented and compared. Crater depth, crater diameter and etching yield are reported versus the laser energy, in order to evaluate the ablation threshold fluence.     

Plasma-mediated ablation of brain tissue with picosecond laser pulses

Plasma-mediated ablations of brain tissue have been performed using picosecond laser pulses obtained from a Nd:YLF oscillator/regenerative amplifier system. The laser pulses had a pulse duration of 35 ps at a wavelength of 1.053 µm. The pulse energy varied from 90 µJ to 550 µJ at a repetition rate of 400 Hz. The energy density at the ablation threshold was measured to be 20 J/cm². Comparisons have been made to 19 ps laser pulses at 1.68 µm and 2.92 µm from an OPG/OPA system and to microsecond pulse trains at 2.94 µm from a free running Er:YAG laser. Light microscopy and scanning electron microscopy were performed to judge the depth and the quality of the ablated cavities. No thermal damage was induced by either of the picosecond laser systems. The Er:YAG laser, on the other hand, showed 20 µm wide lateral damage zones due to the longer pulse durations and the higher pulse energies.     

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.     

Lattice dynamics in two-photon-excited CdS studied by picosecond time-resolved X-ray diffraction

Lattice dynamics and radiative processes in single-crystal cadmium sulfide induced by two-photon excitation with a femtosecond laser are investigated. The development of lattice expansion is directly observed by picosecond time-resolved X-ray diffraction. The obtained lattice dynamics are explained on the basis of a thermally induced impulsive-strain model. The model calculation indicates that two- and more-photon absorption processes occur and that reflectivity rapidly increases under laser irradiation. In photoluminescence spectroscopy, the spectra for TW cm⁻² excitation are shifted to lower energy and show an additional shoulder at 2.35 eV. Furthermore, emission due to Fabry-Perot laser modes with self-formed cavities was observed under 11 TW cm⁻² excitation. The discrepancy between carrier densities deduced from the lattice expansion and the PL spectra indicates that the predominant process at a higher carrier density is not radiative recombination, but Auger recombination followed by lattice heating.     

Spectroscopic characterization of aluminum plasma using laser-induced breakdown spectroscopy

A detailed investigation of aluminum plasma induced by a 1064 nm Nd:YAG laser in air was performed. The emission of spectral lines arising from Al I transition at 396.07 nm, Al II transition at 358.46 nm, Al III transition at 360.72 nm and Al IV transition at 363.05 nm were well-resolved. The plasma parameters including electron temperature and electron density were determined through the Boltzmann plot method using the emission line intensities of the same ionized stages of aluminum atoms and the Stark-broadening profiles of Al II emission line, respectively. The temporal evolutions of the spectral lines belonging to atomic and ionic aluminum elements and the plasma parameters were investigated at three different laser pulse energies. Moreover, the validity of local thermodynamic equilibrium was elucidated in our experimental condition.     

Characterization of laser-generated silicon plasma

A study of visible laser ablation of silicon, in vacuum, by using 3 ns Nd:YAG laser radiation is reported. Nanosecond pulsed ablation, at an intensity of the order of 10¹⁰ W/cm², produces high non-isotropic emission of neutrals and ionic species. Mass quadrupole spectrometry, coupled to electrostatic ion deflection, allows estimation of the energy distributions of the emitted species from plasma. Neutrals show typical Boltzmann-like distributions while ions show Coulomb-Boltzmann-shifted distributions depending on their charge state. Time-of-flight measurements were also performed by using an ion collector consisting of a collimated Faraday cup placed along the normal to the target surface. Surface profiles of the craters, created by the laser radiation absorption, permitted to study the ablation threshold and ablation yields of silicon in vacuum. The plasma fractional ionization, temperature and density were evaluated by the experimental data. A special regard is given to the ion acceleration process occurring inside the plasma due to the high electrical field generated at the non-equilibrium plasma conditions. The angular distribution of the neutral and ion species is discussed.     

Periodic sub-micrometric structures using a 3D laser interference pattern

A method to obtain three-dimensional sub-micrometric periodic structures is presented. The experimental set-up consists in a pulsed UV laser beam source (λ = 355 nm) coming into an interferometer in order to generate four beams converging inside a chamber. According to the directions, to the relative intensities and to the polarizations of these four beams, a 3D interference pattern can be obtained inside the overlapping volume of these four beams; the characteristics of the four laser beams have been optimized in order to obtain a maximal contrast of intensity. In order to visualize the interference pattern, its contrast and its stability at each laser pulse, a video camera coupled to an oil immersion microscope objective has been installed above the interferometer. By suppressing the central beam, it is also possible to generate a bidimensional interference pattern which defines an hexagonal structure in the (1 1 1) plane with a period of 377 nm.This optical set-up has been used to obtain 3D sub-micrometric periodic structures in negative photoresists. Experiments consist in a one- or multi-pulse irradiation of the photoresist followed by a development procedure which leads to a sub-micrometric face-centred cubic structure cut in a (1 1 1) plane with a cell parameter of 650 nm. The optimization of the experimental conditions is presented for two kinds of photoresists; the role of the substrate according to its reflectivity at the laser wavelength and its influence on the interference pattern is also discussed.     

Emission spectra investigation of fs induced NPs probed by the ns laser pulse of a fs/ns DP-LIBS orthogonal configuration

A dual-pulse fs/ns laser induced breakdown spectroscopy configuration, where an initial 250 fs ablating pulsed laser followed by a delayed ns laser beam placed at a fixed distance, orthogonally with the expanding plasma plume, has been used in air on a Al₆₅Cu₂₃Fe₁₂ quasicrystal. The obtained emission data were acquired with a set-up arrangement providing space detections, with a resolution up to 15 μm, of the ns laser pulse generated signals. Assuming the fulfillment of local thermodynamic equilibrium conditions, the role played by the time lag between the two laser beams on the induced plasma excitation temperatures and electronic densities, as well as a space resolved process survey, has been followed. The spatial and time resolved spectra show, almost, steady values of the determined elementary plasma features with the development of nanoparticles occurring during the fs laser pulsed ablation process. The ns laser probe of the dual-pulse LIBS configuration here presented confirms that the nanoparticles induced can be largely widespread in both space and time whose compositions, overall, could retain the starting target stoichiometry. It is shown that these nanoparticles formation can actually take place at different times following the initial ultra-short laser beam incidence and that, especially at long inter-pulse delays (>100 μs), modest compositional changes can be observed.     

Effect of pulse width and fluence of femtosecond laser on the size of nanobump array

Conical nanobump arrays were generated on gold thin film processed by interfering femtosecond laser. The transition of the height and diameter as functions of fluence and pulse width was investigated. When the fluence was 87 mJ/cm², the height and diameter were not so different at 350 fs or shorter pulse width. They decreased at longer pulse width, and no bump could be generated over 1.6 ps. The results suggest the decrease of size is due to the diffusion of electron to not-excited region, and due to heat conduction to not heated region or substrate, or change of absorbance of laser. At long pulse width of 2.4 ps and relatively higher fluence of 190 mJ/cm², nanobump had liquid-like structure as a stop motion of a water drop.     

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.