Emission induced by collision of two plumes during pulsed laser ablation

We observed plume expansion dynamics during pulsed laser ablation when two plumes collided head-on. Si and Ge targets were placed parallel each other, and they were irradiated simultaneously by two pulsed lasers. A new emission appeared near the center of the targets from 250 ns after the irradiation. However, the predominant ejected species is neutral SiI or GeI at this time region when an individual single target is irradiated, and the new emission emerged by collision is a mixture of ionized SiII and GeII. This indicates that the kinetic energy of the collision excites the species to an ionized state. The intensity of this new emission decreased by increasing the background gas pressure. This suggests that collision between two plumes induces a higher-temperature plasma. Since the new emission is composed of ionized Si and Ge species and remains a relatively long period after the collision, this technique will provide a new reactive field to prepare a new kind of alloy nanomaterials.     

Expansion dynamics of the plasma plume created by laser ablation in a background gas

The dynamics of the expansion of the plasma plume induced by laser ablation of a copper target at a fluence of 17 J/cm² was investigated theoretically by means of a Monte Carlo simulation. When the expansion occurs under a relatively high pressure, the ambient gas particles may be involved in the collective motion of the plume. The simulation allows the study of the simultaneous collective motion of different species, such as the laser-ablated and the ambient gas particles. The influence of the background gas nature and pressure on the laser-induced plasma plume expansion behavior was studied. The expansion dynamics were found to be different in the case of the expansion in ambient gases of different molecular weight. The dynamics of the plume expansion under an argon pressure of 200 Pa seem to be strongly related to the equilibration of the pressure gradients in the gas phase, and evidence of the oscillatory behavior of the plume expansion was shown from the evolution over time of the pressure profiles in the plume. This behavior has also been observed in similar conditions for a krypton atmosphere, but for a lower pressure than for argon. The vortical flow formation at the plume periphery, involving both the laser-ablated and the argon particles at moderate pressure, was also predicted from the Monte Carlo simulation.     

Effect of ZnO plasma plume dynamics on laser ablation

The dynamic behaviors and optical properties of a ZnO plasma plume produced by pulsed laser ablation using a Nd:YAG laser (wavelength: 532 nm, pulse width: 3 ns) were studied by fast photography using a commercial gated charge coupled device (CCD) camera linked with a delay circuit and by optical emission spectroscopy at various ambient oxygen pressures. Fast photography was conducted with a resolving power of 0.25 μs and the expansion behaviors of the laser ablation plume were observed. Plasma plume expansion velocity decreased with oxygen partial pressure. The flow of the plasma plume in the early stage of expansion of up to 3 ms agreed well with the drag model.     

Nanoparticle plume dynamics in femtosecond laser ablation of gold

This paper describes some recent results on femtosecond laser ablation of gold. We have studied both the fast vapour/plasma and slow nanoparticle plumes using Langmuir probe, time-resolved ICCD imaging and time-resolved optical absorption measurements. The nanoparticle plume dynamics was analysed by comparing the optical emission absorption measurements with an adiabatic isentropic model of ablation plume expansion, leading to an estimate of the amount of material in the nanoparticle plume.     

Size classification of Si nanoparticles formed by pulsed laser ablation in helium background gas

We have developed an integrated process system for the formation of nanoparticles by pulsed laser ablation (PLA) in helium background gas, size classification using a differential mobility analyzer (DMA), and deposition on a substrate. The DMA has been improved to operate at pressures of less than 10 Torr. The classification resolution of the low-pressure operating DMA (LP-DMA), transporting properties of nanoparticles under low pressure, have been investigated theoretically in order to evaluate the performance of the size classification for the integrated system. By operating the integrated system at less than 10 Torr, we have measured the size distribution of Si nanoparticles in the gas phase formation field by sweeping the applied voltage to the LP-DMA and counting the charged nanoparticle concentration with an electrometer. Moreover, we successfully deposited the classified Si nanoparticles on a substrate by fixing the voltage. We have verified that the integrated system can be applied to the clean physical vapor deposition process for accurately size-controlled nanoparticles.     

Substrate heating effects on the propagation dynamics of laser produced plume during pulsed laser deposition of oxides

We report on the expansion dynamics of laser-produced plasma plumes of complex oxides in an oxygen atmosphere. In particular, we have studied the combined effects of background gas pressure and substrate heating on the plume propagation in typical pressure and temperature regimes of oxides thin film deposition by pulsed laser deposition. Our results evidence a reduced resistance of the background gas to the plume propagation as the substrate temperature increases. The experimental data are analyzed in the frame of a model describing the plume propagation into the background gas. Our experimental findings clearly indicate that the deposition temperature might influence film growth, not only through its direct thermal effect on the surface kinetics of adatoms, but also by affecting the energetic properties of the precursors in the gas phase.     

Measurement of Er:YAG laser ablation plume dynamics

The dynamics of tissue ablation using an Er:YAG laser were studied using flash photography and optical pump-probe techniques. Both normal-spiking-mode and Q-switched Er:YAG laser radiation were used to study the ablation of skin and bone. Time-resolved photographs of the ablation plume were obtained using a microscope-mounted camera together with pulsed illumination from an excimer-pumped dye laser. The velocity of the plume front, obtained from the photographs, was approximately 1400 m/s. The same velocity was also measured using an optical pump-probe technique. Both techniques indicate that material removal occurred after the end of the 90-ns-long Q-switched laser pulse and that each micropulse in the normal-spiking-mode pulse train was capable of ablating and rapidly ejecting tissue.This work was supported in part by the SDIO-MFEL Program under contract # N00014-86-K-0117 and by the Arthur O. and Gullan M. Wellman Foundation     

Plume dynamics during film and nanoparticles deposition by pulsed laser ablation

The gas dynamics of pulsed laser ablation of silicon target in the helium gas ambient is investigated via direct simulation Monte Carlo method with a real physical scale of target-substrate configuration. A shock driven process is clearly observed. It is shown that the interaction of the shock front with the target surface and the vapor front induce significant backward flux of ablated particles and oscillating behavior of vapor front. A confined layer mixed with high density Si and He atoms is formed around the contact front. Its behavior is important to the nanoparticle formation and deposition.     

Plasma plume induced during laser ablation of graphite

The plasma plume induced during ArF laser ablation of a graphite target is studied. Velocities of the plasma expansion front are determined by the optical time of flight method. Mass center velocities of the emitting atoms and ions are constant and amount to 1.7×10⁴ and 3.8×10⁴ m s⁻¹, respectively. Higher velocities of ions result probably from their acceleration in electrostatic field created by electron emission prior to ion emission. The emission spectroscopy of the plasma plume is used to determine the electron densities and temperatures at various distances from the target. The electron density is determined from the Stark broadening of the Ca II and Ca I lines. It reaches a maximum of ∼9.5×10²³ m⁻³ 30 ns from the beginning of the laser pulse at the distance of 1.2 mm from the target and next decreases to ∼1.2×10²² m⁻³ at the distance of 7.6 mm from the target. The electron temperature is determined from the ratio of intensities of ionic and atomic lines. Close to the target the electron temperature of ∼30 kK is found but it decreases quickly to 11.5 kK 4 mm from the target.     

Molecular dynamics study of nanoparticle evolution in a background gas under laser ablation conditions

Long-time evolution of nanoparticles produced by short laser interactions is investigated for different materials. To better understand the mechanisms of the nanoparticle formation at a microscopic level, we use molecular dynamics (MD) simulations to analyse the evolution of a cluster in the presence of a background gas with different parameters (density and temperature). In particular, we compare the simulation results obtained for materials with different interaction potentials (Morse, Lennard-Jones, and Embedded Atom Model). Attention is focused on the evaporation and condensation processes of a cluster with different size and initial temperature. As a result of the MD calculations, we determinate the influence of both cluster properties and background gas parameters on the nanoparticle evolution. The role of the interaction potential is discussed based on the results of the simulations.     

Modeling of plume dynamics with shielding in laser ablation of carbon

The process of laser ablation of carbon in presence of background gas is simulated numerically. The plume dynamics in laser ablation is important to study for many reasons including temperature of plume particles and shielding of target by previously ablated plumes. Shielding leads directly to the change in energy deposition of incident laser pulse at the target surface and in turn influences the ablation dynamics and amount of material removed. Carbon ablation is studied for single and multiple laser hits typical for synthesis of nanotubes. Two models of correction of ablated velocity and pressure resulting from shielding effect are proposed and investigated. Numerical modeling of this plume dynamics and its integral effect of shielding is challenging due to inherent high nonlinearity of the problem. Some of available numerical techniques handles nonlinearity but are dissipative, e.g. Godunov type schemes. Other techniques are less dissipative but fail to account for strong nonlinearity typical for initial stages of ablation, e.g. the ENO-Roe. To effectively model this highly nonlinear plume dynamics a combination of two of above mentioned schemes is developed so as the numerical evaluation of fluxes is close to their physical values and the scheme has minimum dissipation. The non-monotonic behavior of ablated mass as a function of time duration between two laser pulses is studied.     

Structural and optical properties of silicon nanoparticles prepared by pulsed laser ablation in hydrogen background gas

We studied the structural and optical properties of silicon (Si) nanoparticles (np-Si) prepared by pulsed laser ablation (PLA) in hydrogen (H₂) background gas. The mean diameter of the np-Si was estimated to be approximately 5 nm. The infrared absorption corresponding to Si-H_n (n=1,2,3) bonds was observed at around 2100 cm^-1, and a Raman scattering peak corresponding to crystalline Si was observed at around 520 cm^-1. These results indicate that nanoparticles are not an alloy of Si and hydrogen but Si nanocrystal covered by hydrogen or hydrogenated silicon. This means that surface passivated Si nanoparticles can be prepared by PLA in H₂ gas. The band-gap energy of np-Si prepared in H₂ gas (1.9 eV) was larger than that of np-Si prepared in He gas (1.6 eV) even though they are almost the same diameter. After decreasing the hydrogen content in np-Si by thermal annealing, the band-gap energy decreased, and reached the same energy level as np-Si prepared in He gas. Thus, the optical properties of np-Si were affected by the hydrogenation of the surface of np-Si. PACS 81.15.Fg; 61.46.+W; 78.67.Bf     

Background gas collisional effects on expanding fs and ns laser ablation plumes

The collisional effects of a background gas on expanding ultrafast and short pulse laser ablation plumes were investigated by varying background pressure from vacuum to atmospheric pressure levels. For producing Cu ablation plumes, either 40 fs, 800 nm pulses from a Ti: Sapphire laser or 6 ns, 1,064 nm pulses from a Nd:YAG laser were used. The role of background pressure on plume hydrodynamics, spectral emission features, absolute line intensities, signal to background ratios and ablation craters was studied. Though the signal intensities were found to be maximum near to atmospheric pressure levels, the optimum signal to background ratios are observed ~20–50 Torr for both ns and fs laser ablation plumes. The differences in laser–target and laser–plasma couplings between ns and fs lasers were found to be more engraved in the crater morphologies and plasma hydrodynamic expansion features.     

Correlation of plume dynamics and oxygen pressure with VO2 stoichiometry during pulsed laser deposition

Vanadium dioxide thin films have been deposited on Corning glass substrates by a KrF laser ablation of V₂O₅ target at the laser fluence of 2 J?cm^?2. The substrate temperature and the target-substrate distance were set to 500 ^°C and 4 cm, respectively. X-ray diffraction analysis showed that pure VO₂ is only obtained at an oxygen pressure range of 4×10^?3–2×10^?2 mbar. A higher optical switching contrast was obtained for the VO₂ films deposited at 4×10^?3–10^?2 mbar. The films properties were correlated to the plume-oxygen gas interaction monitored by fast imaging of the plume.     

Numerical study of ultra-short laser ablation of metals and of laser plume dynamics

Numerical modeling is used to investigate the physical mechanisms of the interaction of ultra-short (sub-picosecond) laser pulses with metallic targets. The laser–target interaction is modeled by using a one-dimensional hydrodynamic code that includes the absorption of laser radiation, the electronic heat conduction, the electron-phonon or electron–ion energy exchange, as well as a realistic equation of state. Laser fluences typical for micromachining are considered. The results of the 1D modeling are then used as the initial conditions for a 2D plasma expansion model. The dynamics of laser plume expansion in femtosecond regime is investigated. Calculations show that the plasma plume is strongly forward directed. In addition, a two-peaked axial density profile is obtained for 400 nm laser wavelength. The calculation results agree with the experimental observations. PACS 52.38.Mf; 02.60.Cb