Plume Expansion Dynamics Research Articles

Effects of oxygen background pressure on the stoichiometry of a LaGaO3 laser ablation plume investigated by time and spectrally resolved two-dimensional imaging

The plume expansion dynamics strongly affects the growth and the chemistry of pulsed laser deposited thin films. The interaction with the background gas determines the kinetic energy of the species impinging on the substrate, their angular broadening, the plasma chemistry, and eventually the cations stoichiometric ratio in oxide films. Here, we exploit two-dimensional, spectrally resolved plume imaging to characterize the diverse effects of the oxygen background pressure on the expansion dynamics of La, Ga, and LaO species during pulsed laser deposition of LaGaO3. The propagation of the ablated species towards the substrate is studied for background oxygen pressures ranging from high vacuum up to ≈10−1 mbar. Our experimental results show specie-dependent effects of the background gas on the angular distribution of the precursors within the plume. These findings suggest that even in the presence of a stoichiometric ablation and of a globally stoichiometric plume, cations off-stoichiometry can take place in the forefront portion of the plume impinging on the substrate. We show that such effect can be compensated by a proper choice of process parameters.

The Effect of an External Magnetic Field on the Plume Expansion Dynamics of Laser-Induced Aluminum Plasma**supported by National Natural Science Foundation of China (No. 61178022), the Research Foundation for Doctoral Program of Higher Education of China (Nos. 20112216120006, 20122216120009 and 20122216110007) and also the Project of 14KP007

In this work, we investigated the plasma morphology induced by a Nd:YAG laser with the aim of improving the understanding of the formation and dynamics of the plasma in two cases, with and without a magnetic field. Single laser pulse production of a plasma in the absence and presence of a magnetic field was performed with an aluminum target in air. A fast photography technique was employed to obtain information about the expansion dynamics and confinement of the aluminum plasma in each case. The generation of the laser plasma was allowed to expand at two locations with different magnetic field strengths, which correspond to the strength 0.58 T in the center of two magnetic poles and 0.83 T at a distance of 4 mm from the upper pole (N). The plume showed lateral confinement at longer delays when the target was placed at the center of the two poles. When the target was placed at a distance of 4 mm from the upper pole it was observed that the plume was divided into two lobes at the initial stage and traveled towards the center of the magnetic field with further elapse of time.

Ablation plume structure and dynamics in ambient gas observed by laser-induced fluorescence imaging spectroscopy

The dynamic behavior of an ablation plume in ambient gas has been investigated by laser-induced fluorescence imaging spectroscopy. The second harmonic beam from an Nd:YAG laser (0.5–6J/cm2) was focused on a sintered oxide pellet or a metal chip of gadolinium. The produced plume was subsequently intersected with a sheet-shaped UV beam from a dye laser so that time-resolved fluorescence images were acquired with an intensified CCD camera at various delay times. The obtained cross-sectional images of the plume indicate that the ablated ground state atoms and ions of gadolinium accumulate in a hemispherical contact layer between the plume and the ambient gas, and a cavity containing a smaller density of ablated species is formed near the center of the plume. At earlier expansion stage, another luminous component also expands in the cavity so that it coalesces into the hemispherical layer. The splitting and coalescence for atomic plume occur later than those for ionic plume. Furthermore, the hemispherical layer of neutral atoms appears later than that of ions; however, the locations of the layers are nearly identical. This coincidence of the appearance locations of the layers strongly suggests that the neutral atoms in the hemispherical layer are produced as a consequence of three-body recombination of ions through collisions with gas atoms. The obtained knowledge regarding plume expansion dynamics and detailed plume structure is useful for optimizing the experimental conditions for ablation-based spectroscopic analysis.

On the relevance of large scale pulsed-laser deposition: Evidence of structural heterogeneities in ZnO thin films

Pulsed-laser deposition is known as a well-suited method for growing thin films of oxide compounds presenting a wide range of functional properties. A limitation of this method for industrial process is the very anisotropic expansion dynamics of the plasma plume, which induces difficulties to grow on large scale films with homogeneous thickness and composition. The specific aspect of the crystalline or orientation uniformity has not been investigated, despite its important role on oxide films properties. In this work, the crystalline parameters and the texture of zinc oxide films are studied as a function of position with respect to the central axis of the plasma plume. We demonstrate the existence of large non-uniformities in the films. The stoichiometry, the lattice parameter, and the distribution of crystallites orientations drastically depend on the position with respect to the plume axis, i.e., on the oblique incidence of the ablated species. The origin of these non-uniformities, in particular, the unexpected tilted orientation of the ZnO c-axis may be attributed to the combined effects of the oblique incidence and of the ratio between oxygen and zinc fluxes reaching the surface of the growing film.

Experimental investigation of plume expansion dynamics of nanosecond laser ablated Al with small incident angle

Experimental study of expansion dynamics of pulsed-laser ablation plasmas from Al is presented. A systematic investigation of plasma plume expansion is done. The laser beam is focused on the target with an incident angle between 0° and 20°. The results show that the plume growth is almost normal to the target surface, irrespective of the incident angle of the laser. Besides, the time evolution of the plasma plume geometry ratio at different incident angles shows that the incident angle of laser beam influences very slightly its shape at later delay time. The results imply that when the incident angle is small (ranging from 0° to 20°), the influence of the incident angle on the plume expansion is rather trivial.

Emission features and expansion dynamics of nanosecond laser ablation plumes at different ambient pressures

The influence of ambient pressure on the spectral emission features and expansion dynamics of a plasma plume generated on a metal target has been investigated. The plasma plumes were generated by irradiating Cu targets using 6 ns, 1064 nm pulses from a Q-switched Nd:YAG laser. The emission and expansion dynamics of the plasma plumes were studied by varying air ambient pressure levels ranging from vacuum to atmospheric pressure. The ambient pressure levels were found to affect both the line intensities and broadening along with the signal to background and signal to noise ratios and the optimum pressure conditions for analytical applications were evaluated. The characteristic plume parameters were estimated using emission spectroscopy means and noticed that the excitation temperature peaked ∼300 Torr, while the electron density showed a maximum ∼100 Torr. Fast-gated images showed a complex interaction between the plume and background air leading to changes in the plume geometry with pressure as well as time. Surface morphology of irradiated surface showed that the pressure of the ambient gas affects the laser-target coupling significantly.

Plume dynamics of a laser produced plasma from a dot target

To generate a plasma light source with a small spot size by reducing the expansion of the plasma plume, we studied the plume expansion dynamics of a plasma generated from a dot target that consisted of a photoresist with a hole coated on a pure Al plate. A time-resolved ultraviolet (UV) image of the plasma plume and a UV spectrometer were used to study the expansion of the plasma plume produced from a dot target and from an Al plate target. The measurements of the plume size from the emission of Al II ions showed that due to the strong collision between the core Al plasma and the plasma generate from the outer part of the dot, the expansion speed in the lateral direction was reduced to 70 % that of the plasma generated from the pure Al plate. However, for the case of the emission from neutral Al atoms, the plume sizes of the two targets were almost the same because of the weak collision between the Al atoms and the surrounding plasmas. Thus, these collisional effects in the plasma produced from a dot target can reduce the size of the core plasma ion and can be used to generate a small-spot-size laser plasma light source.

Fluid simulation of plume head-on collision dynamics during pulsed laser ablation

Expansion dynamics of plume after irradiation of the target material is essential to prepare nanoparticles by pulsed laser ablation and it can be modified by collision of two plumes. In the present paper, effect of head-on collision on the expansion dynamics is discussed by numerical simulation based on the fluid dynamics and compared with the experimental results of plume emission. Suppression of plumes by collision with counter plume observed by experiment is reproduced by numerical simulation. Results of the numerical calculation indicate that shockwave induced by the irradiation of the opposite target suppress vapor expansion. The vapors do not mix around the center of the targets when the two targets are irradiated simultaneously and unstable flow is seen when delay between laser pulses was applied for irradiation of two targets. The results of the numerical simulation suggest that formation of combined and alloy nanoparticles are expected for former and latter cases.

Fabrication of Nano-engineered Transparent Conducting Oxides by Pulsed Laser Deposition

Nanosecond Pulsed Laser Deposition (PLD) in the presence of a background gas allows the deposition of metal oxides with tunable morphology, structure, density and stoichiometry by a proper control of the plasma plume expansion dynamics. Such versatility can be exploited to produce nanostructured films from compact and dense to nanoporous characterized by a hierarchical assembly of nano-sized clusters. In particular we describe the detailed methodology to fabricate two types of Al-doped ZnO (AZO) films as transparent electrodes in photovoltaic devices: 1) at low O₂ pressure, compact films with electrical conductivity and optical transparency close to the state of the art transparent conducting oxides (TCO) can be deposited at room temperature, to be compatible with thermally sensitive materials such as polymers used in organic photovoltaics (OPVs); 2) highly light scattering hierarchical structures resembling a forest of nano-trees are produced at higher pressures. Such structures show high Haze factor (>80%) and may be exploited to enhance the light trapping capability. The method here described for AZO films can be applied to other metal oxides relevant for technological applications such as TiO₂, Al₂O₃, WO₃ and Ag₄O₄.

Diagnostics of nonuniform plasmas for elemental analysis via laser-induced breakdown spectroscopy: demonstration on carbon-based materials

We investigate the plasma produced by the interaction of ultraviolet nanosecond laser pulses with a carbon fiber composite tile from the inner wall of a fusion reactor. The experiments are carried out in argon at a pressure of 5 × 104 Pa. Fast imaging is used to characterize the plume expansion dynamics and excited plasma species are followed by time- and space-resolved emission spectroscopy. The measurements show that ionized and highly excited plasma species are located in the front of the expanding plume, whereas neutral atoms and lower excited species dominate in the plasma core. By measuring the excitation temperature of metallic ions and neutral atoms, we evidence the existence of a temperature gradient that appears during the early expansion stage and remains up to delays typically used in material analysis via laser-induced breakdown spectroscopy. The knowledge of the spatial distribution of the plasma properties is then used to model the plasma emission spectrum. Assuming two plasma zones in local thermodynamic equilibrium of different temperatures and electron densities, we calculate the spectral radiance and compare it to the spatially integrated spectrum recorded with an Echelle spectrometer. From the best agreement between measured and computed spectra we deduce the elemental concentrations of carbon, hydrogen and metal impurities. The validity of the model is critically discussed and the measurement uncertainties are evaluated. The present approach is foreseen to improve the accuracy of analysis via laser-induced breakdown spectroscopy in many applications, in particular when materials of elements with significantly different ionization potentials are investigated.

Fast imaging of the laser-blow-off plume driven shock wave: Dependence on the mass and density of the ambient gas

Abstract A systemic investigation of expansion dynamics of plasma plume, produced by laser-blow-off of LiF–C thin film has been done with emphasis on the formation of shock wave and their dependence on the pressure and nature of the ambient gas. The present results demonstrate that highly directional plume produces a strong shock wave in comparison to shock produced by the diverging plume. Shock-velocity, strength and its structure are strongly dependent on ambient environment; maximum shock velocity is observed in helium whereas shock strength is highest in argon environment. The role of chemically reactive processes was not observed in the present case as the plume structure is almost similar in argon and oxygen.

On Predtechensky and Mayorov model for the plume expansion dynamics study into an ambient gas during thin film deposition by laser ablation

The plume expansion dynamics for the Sm1−x Nd x NiO3 thin films deposition by a KrF excimer laser into oxygen atmosphere has been investigated using fast imaging. The study was carried out at 0.2 and 0.3 mbar of oxygen pressure and for different laser fluences. The plasma plume dynamics was analysed in the framework of Predtechensky and Mayorov (PM) model. It was found that PM model gives a general description of the plume expansion by using parameters (laser fluence and oxygen pressure) that ensure a hemispherical expansion of the plume. The latter was discussed in the framework of the shock-wave model and the plume dimensions.

Effects of collision between two plumes on plume expansion dynamics during pulsed laser ablation in background gas

Si and Ge targets were simultaneously irradiated by individual two pulsed lasers, and two plumes from the targets were collided head-on with expectation to prepare hybrid nanoparticles. We investigate effects of He background gas pressure on plume collision dynamics. Three characteristic behaviors of plume expansion dynamics are observed at low, middle, and high background gas pressure regions. Interaction between the two atomic species during plume expansion was small and the effect of collision was hardly observed at a low background gas pressure, 130 Pa, while spatial evolution of the plume was suppressed at middle pressure, 270 Pa, due to collision of the two plumes. At high pressure, 2700 Pa, plume expansion is suppressed by background gas and the effect of a direct collision of two plumes was small. These results indicate that plume collision dynamics, which governs nanoparticle formation, and the mixture of Si and Ge species can be varied by background gas pressure. The deposit near the center of two targets was nanoparticles that were composed of Si and Ge.

Oxygen background gas influence on pulsed laser deposition process of LaAlO3 and LaGaO3

We investigate pulsed laser ablation of LaAlO3 and LaGaO3 with a focus on the influence of oxygen background gas pressure on the plume expansion dynamics and deposition rate. The ablation plume is characterized by exploiting fast photography and time- and space-resolved optical emission spectroscopy. The variation of the deposition rate with the oxygen background pressure was obtained at 800°C by reflection high-energy electron diffraction, and compared to that measured at room temperature by means of a quartz crystal microbalance. The experimental findings allow one to address the various stages of plume expansion as a function of the background oxygen pressure as well as the changes induced on the plume species kinetic energy and composition. On the base of our experimental results, the possible influence of various mechanisms, such as subplantation and oxygen vacancy formation, on the growth of oxides interfaces is addressed.

Effect of Argon Ambient Gas Pressure on Plume Expansion Dynamics

In this paper we present a numerical modeling of a nanosecond laser pulse interaction with a titanium target. We investigate the vapor plume formation and the influence of the ambient gas pressure on plume expansion dynamics. The vapor plume formation depends on the results of the heat transfer in the solid target modeling. The solid-liquid phase change is modeled by a two dimensional approach using an enthalpy formulation. The resulting plume expansion in the argon background gas is studied using the species transport model. The algebraic equations are discretized by the finite volume method implemented by Fluent CFD software [1]. The calculation results of plume expansion velocity, density, temperature and degree of ionization in the plume are presented.

Characterization of Laser Induced Plasmas by Fast Imaging for Graphite Target

Plume expansion dynamics of an ablated graphite target by the third harmonic of Nd-YAG laser of 355 nm wavelength has been investigated using an ICCD camera fast imaging. This study was carried out into vacuum and methane (CH4) atmosphere at different pressures. Into vacuum, the two dimensional spatio-temporal evolution of plasma plume was performed at a laser irradiance range of 5.5x108 - 6x109 W/cm2. The plasma mean velocity has been estimated and was found to increase with laser power density increases until it reaches a maximum value of 107 cm/s. In presence of gas, the plasma plume dynamics was studied at a fixed irradiance of 4.3x 109 W/cm2 and from 0.05 to 5 mbar CH4 pressures. The plasma spatio-temporal evolution was found to be influenced by the gas pressure. In earlier time the expansion was almost linear independently of the background gas pressure used. However, as time evolves, the plume is decelerated, then presented a stationary behaviour at 1 and 5 mbar. Furthermore, the light emission from the plume very close to the target surface exists until a few microseconds into vacuum and CH4 atmosphere and then vanishes. It appears again around 10 µs following by the emission of particulates as bright incandescent tracks.

Investigation of plasmas produced by laser ablation using single and double pulses for food analysis demonstrated by probing potato skins

We report on investigations of plasmas produced by laser ablation of fresh potatoes using infrared nanosecond laser radiation. A twin laser system consisting of two Nd:YAG oscillators was used to generate single or double pulses of adjustable interpulse delay. The potatoes were irradiated under ambient air with moderate pulse energies of about 10 mJ. The expansion dynamics of the ablation plume was characterized using fast imaging with a gated camera. In addition, time-resolved optical emission spectroscopy was applied to study the spectral line emission of the various plasma species. The electron density was deduced from Stark broadening, and the plasma temperature was inferred from the relative emission intensities of spectral lines. The relative concentrations of metals were estimated from the comparison of the measured emission spectra to the spectral radiance computed for a plasma in local thermal equilibrium. It is shown that the plasma produced by double pulses has a larger volume and a lower density. These properties lead to an increase of the signal-to-noise ratio by a factor of 2 and thus to an improved measurement sensitivity.

The effect of excitation wavelength on dynamics of laser-produced tin plasma

We investigated the effect of the excitation wavelength on the density evolution of laser-produced tin plasmas, both experimentally and numerically. For producing plasmas, Sn targets were excited with either 10.6 μm CO2 laser or 1.06 μm Nd:yttrium aluminum garnet laser; both are considered to be potential excitation lasers for extreme ultraviolet lithography laser-produced plasma light sources. The electron density of the plasma during the isothermal expansion regime was estimated using an interferometric technique. The Stark broadening of isolated singly-ionized emission was employed for deducing the density during the plasma adiabatic expansion regime. Our results indicate that the excitation source wavelength determines the initial density of the plasma, as well the plume expansion dynamics. Numerical simulation using HEIGHTS simulation package agrees well with the experimentally measured density profile.

Ultra-fast laser ablation and deposition of TiO2

In this work we report on the properties of the ablation plume and the characteristics of the films produced by ultra-fast pulsed laser deposition (PLD) of TiO2 in vacuum. Ablation was induced by using pulses with a duration of ≈300 fs at 527 nm. We discuss both the composition and the expansion dynamics of the TiO2 plasma plume, measured by exploiting time- and space-resolved emission spectroscopy and gated imaging. The properties of the TiO2 nanoparticles and nanoparticle-assembled films were characterized using different techniques, i.e. environmental scanning electron microscopy (ESEM), atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS). It is suggested that most of the material decomposes in the form of nanoparticles.

Characterization of aerosol plumes in nanosecond laser ablation of molecular solids at atmospheric pressure

Ablation of molecular solids with pulsed ultraviolet lasers at atmospheric pressure is an important process in (bio-)organic mass spectrometry. Of practical importance for analytical sampling and analysis are the plume formation and expansion. Plumes formed by atmospheric-pressure laser ablation of anthracene and 2,5-dihydroxybenzoic acid (2,5-DHB) were studied by light scattering imaging, which showed significant material release in the form of aerosols. The monitored plume expansion dynamics could be fitted to the drag-force model, yielding initial plume velocities of 150 m/s for anthracene and 43 m/s for DHB. While the angle of incidence does not affect the plume direction and propagation, a large dependence of the plume-expansion velocity on the laser pulse energy could be found, which is limited at atmospheric pressure by the onset of plasma shielding. With respect to analytical applications, the efficiency of sampling of the laser ablation products by a capillary could be experimentally visualized.