Ablation Plume Research Articles

An analytical continuum-based model of time-of-flight distributions for pulsed laser ablation

An analytical model for time-of-flight (TOF) distributions of particles produced by pulsed laser ablation in vacuum has been proposed. The model takes into account the hydrodynamic expansion stage of the ablation plume and is based on a ‘sudden freeze’ model developed previously for steady-state supersonic jets. It is assumed that a continuum-like expansion of the plume takes place until a freezing time moment t free (or, alternatively, until a ‘freezing distance’ x free) whereupon the collisionless expansion begins. The proposed model is applied for analysis of experimental data on graphite ablation with nanosecond laser pulses. For verification, the analytical distributions are compared with calculated results obtained using a hybrid model combining a thermal model of laser-induced material heating with calculations of the plume dynamics by the direct simulation Monte Carlo (DSMC) method. It is shown that the proposed model can accurately estimate the surface temperature for conditions when the common approach fails.

Morphological evaluation of hard tissues irradiated by holmium laser under various environments using optical coherence microscopy

In order to investigate the influence of water environment on fiber-guided holmium laser ablation of hard tissues, high-speed photography is performed to accurately record the dynamic evolutions of vaporization bubbles and ablation plumes, and optical coherence microscopy is also used to measure the crater morphology. Experimental results indicate that under the same condition, the ablation performances in air and in water for a single long-pulse laser are comparable when the used fibers are in perpendicular contact with the tissues. But for multiple-pulses ablation, the ablation performances such as ablation efficiency and surface morphology in water become better than those in air because of more and more significant vaporization effect for bigger ablation craters. Optical coherence microscopy is an effective tool for the morphological measurement of craters.

The origin of the metal enrichment of carbon nanostructures produced by laser ablation of a carbon–nickel target

Compositional analysis of metal-containing carbon thin films and nanostructures produced by pulsed laser ablation of a carbon–nickel target revealed significantly higher fractions of nickel in the materials than in the target used to produce them. Ablation of mixed targets is used routinely in the synthesis of carbon nanotubes and to enhance the conductivity of amorphous carbon films by metal incorporation. In this extensive study we investigate the physical mechanisms underlying this metal-enrichment and relate changes in the dynamics of the ablation plumes with increasing background gas pressure to the composition of deposited materials. The failure to preserve the target atom ratios cannot, in this case, be attributed to conventional mechanisms for non-stoichiometric transfer. Instead, nickel-enrichment of the target surface by back-deposition, combined with significantly different propagation dynamics for C atoms, Ni atoms and alloy clusters through the background gas, appears to be the main cause of the high nickel fractions.

Experimental and computational study of complex shockwave dynamics in laser ablation plumes in argon atmosphere

We investigated spatio-temporal evolution of ns laser ablation plumes at atmospheric pressure, a favored condition for laser-induced breakdown spectroscopy and laser-ablation inductively coupled plasma mass-spectrometry. The 1064 nm, 6 ns pulses from a Nd:YAG laser were focused on to an Al target and the generated plasma was allowed to expand in 1 atm Ar. The hydrodynamic expansion features were studied using focused shadowgraphy and gated 2 ns self-emission visible imaging. Shadowgram images showed material ejection and generation of shock fronts. A secondary shock is observed behind the primary shock during the time window of 100-500 ns with instabilities near the laser cone angle. By comparing the self-emission images obtained using fast photography, it is concluded that the secondary shocks observed in the shadowgraphy were generated by fast moving target material. The plume front estimates using fast photography exhibited reasonable agreement with data obtained from shadowgraphy at early times ≤400 ns. However, at later times, fast photography images showed plume confinement while the shadowgraphic images showed propagation of the plume front even at greater times. The structure and dynamics of the plume obtained from optical diagnostic tools were compared to numerical simulations. We have shown that the main features of plume expansion in ambient Ar observed in the experiments can be reproduced using a continuum hydrodynamics model which provided valuable insight into the expansion dynamics and shock structure of the plasma plume.

Laser opto-acoustic study of phase transitions in metals confined by transparent dielectric

First-order phase transitions in metal induced by nanosecond laser pulse are studied here. The metal surface is irradiated through a layer of transparent dielectric—an optical glass. Such confinement considerably increases the efficiency of pressure generation at the metal surface. This technique allows to obtain near-critical states of metals—with temperatures ∼104 K and pressures ∼104 atm with table-top equipment. At the same time the glass prevents the ablation plume formation—so the surface temperature can be measured using thermal radiation data. An experimental setup for simultaneous measurements of pressure, temperature and reflectivity was assembled based on the elaborated method of experimental research. The processes of melting of lead and boiling of mercury were studied. The onset of the phase transition process led to a considerable tightening of the pressure pulse. A substantial drop of surface reflectivity due to increase of temperature and decrease of density was observed.

Plasma plume effects on the conductivity of amorphous-LaAlO3/SrTiO3 interfaces grown by pulsed laser deposition in O2 and Ar

Amorphous-LaAlO3/SrTiO3 interfaces exhibit metallic conductivity similar to those found for the extensively studied crystalline-LaAlO3/SrTiO3 interfaces. Here, we investigate the conductivity of the amorphous-LaAlO3/SrTiO3 interfaces grown in different pressures of O2 and Ar background gases. During the deposition, the LaAlO3 ablation plume is also studied, in situ, by fast photography and space-resolved optical emission spectroscopy. An interesting correlation between interfacial conductivity and kinetic energy of the Al atoms in the plume is observed: to assure conducting interfaces of amorphous-LaAlO3/SrTiO3, the kinetic energy of Al should be higher than 1 eV. Our findings add further insights on mechanisms leading to interfacial conductivity in SrTiO3-based oxide heterostructures.

Application of time-resolved digital holographic microscopy in studies of early femtosecond laser ablation

We studied evolution of femtosecond laser ablation by employing novel method of time-resolved off-axis digital holographic microscopy. Phase and amplitude profiles of early shock front and ablation plume dynamics of irradiated tempered steel were reconstructed from the digital holograms. In order to gain additional information, digital holographic microscopy was combined with plasma emission imaging. By using both techniques simultaneously we studied material response to multi-pulse irradiation, shock wave propagation, ablation plume formation and plasma emission. The significant changes in ablation performance were observed when using multi-pulse irradiation if compared to widely investigated single-shot regime.

Influence of water environment on holmium laser ablation performance for hard tissues

This study clarifies the ablation differences in air and in water for hard biological tissues, which are irradiated by fiber-guided long-pulsed holmium lasers. High-speed photography is used to record the dynamic characteristics of ablation plumes and vaporization bubbles induced by pulsed holmium lasers. The ablation morphologies and depth of hard tissues are quantitatively measured by optical coherence microscopy. Explosive vaporization effects in water play a positive role in the contact ablation process and are directly responsible for significant ablation enhancement. Furthermore, water layer depth can also contribute to ablation performance. Under the same laser parameters for fiber-tissue contact ablation in air and water, ablation performances are comparable for a single-laser pulse, but for more laser pulses the ablation performances in water are better than those in air. Comprehensive knowledge of ablation differences under various environments is important, especially in medical procedures that are performed in a liquid environment.

Accumulation of air in polymeric materials investigated by laser-induced breakdown spectroscopy

We report on spectroscopic analyses of plasmas produced by laser irradiation of nitrogen-free and nitrogen-containing polymer materials. Ultraviolet laser pulses of 5 ns duration and 4 mJ energy were focused onto the samples with a fluence of about 20 Jcm−2. The plasma emission was analyzed with an Echelle spectrometer equipped with a gated detector. Comparing the spectra recorded during ablation in air and argon, it is shown that the spectral line emission of atomic nitrogen originates from the excitation of the ambient air, whereas the CN molecular bands are essentially emitted from the ablation plume. Furthermore, the measurements demonstrate an additional contribution of nitrogen emission from the air molecules accumulated in the polymer. Storage under vacuum over a duration of the order of one day leads to the release of the absorbed air. As a consequence of the air absorption, the measurement of elemental composition of polymers via laser-induced breakdown spectroscopy is particularly difficult. Here, we quantify the atmospheric contribution to the plume emission during polymer analysis.

Estimation of the absorptivity of a constructive material at unknown losses in ablation plume during laser ablation

Computation of the processes of laser heating of carbon silicon carbide composite material (CSCCM) samples in air (to temperatures above 2000°C for 1 s) by IR laser radiation with a wavelength of 1.3 µm and intensity of 3 kWcm−2 in the presence of screening ablation plume have been carried out using the KARAT code. A comparison of the simulation results with the experimental dependences of spatial and temporal fields of sample temperatures made it possible to determine the absorptivity of thematerial, energy loss in the ablation plume, and, correspondingly, its influence on the heating and ablation of the material under study.

Analysis of the sizes and number of microparticles in the ablation plume, which attenuates laser radiation during ablation of a constructive material

The effect of laser radiation with a wavelength of 1.3 µm, power of 25 kW, pulse width of 1 s, and irradiated spot area of 9 cm2 on carbon silicon carbide composite material (CSCCM) is analyzed. The formation of an ablation plume (which consists of vapor of irradiated material, burning products, drops and microparticles of various chemical composition and size) above the irradiated surface leads to a significant loss of laser energy. The fractions of the scattered and absorbed laser radiation in the plume are determined, the size and mass distributions of microparticles in the plume are estimated, their concentration is calculated, and the microparticle escape velocities from the irradiated CSCCM surface are evaluated.

Laser ablation loading of a radiofrequency ion trap

The production of ions via laser ablation for the loading of radiofrequency (RF) ion traps is investigated using a nitrogen laser with a maximum pulse energy of 0.17 mJ and a peak intensity of about 250 MW/cm^2. A time-of-flight mass spectrometer is used to measure the ion yield and the distribution of the charge states. Singly charged ions of elements that are presently considered for the use in optical clocks or quantum logic applications could be produced from metallic samples at a rate of the order of magnitude 10^5 ions per pulse. A linear Paul trap was loaded with Th+ ions produced by laser ablation. An overall ion production and trapping efficiency of 10^-7 to 10^-6 was attained. For ions injected individually, a dependence of the capture probability on the phase of the RF field has been predicted. In the experiment this was not observed, presumably because of collective effects within the ablation plume.

Enhanced high-order-harmonic generation in a carbon ablation plume

We report on the observation of enhanced high harmonics from a carbon plasma using sub-5-fs laser pulses. The efficiency of harmonic generation in the range of 14--25 eV was up to five times higher in the case of a plasma medium (graphite ablation) compared with gas (argon) under similar experimental conditions. The harmonic enhancement can be attributed to the presence of carbon nanoparticles in the ablation plumes.

Infrared Laser Ablation Atmospheric Pressure Photoionization Mass Spectrometry

In this paper we introduce laser ablation atmospheric pressure photoionization (LAAPPI), a novel atmospheric pressure ion source for mass spectrometry. In LAAPPI the analytes are ablated from water-rich solid samples or from aqueous solutions with an infrared (IR) laser running at 2.94 μm wavelength. Approximately 12 mm above the sample surface, the ablation plume is intercepted with an orthogonal hot solvent (e.g., toluene or anisole) jet, which is generated by a heated nebulizer microchip and directed toward the mass spectrometer inlet. The ablated analytes are desolvated and ionized in the gas-phase by atmospheric pressure photoionization using a 10 eV vacuum ultraviolet krypton discharge lamp. The effect of operational parameters and spray solvent on the performance of LAAPPI is studied. LAAPPI offers ~300 μm lateral resolution comparable to, e.g., matrix-assisted laser desorption ionization. In addition to polar compounds, LAAPPI efficiently ionizes neutral and nonpolar compounds. The bioanalytical application of the method is demonstrated by the direct LAAPPI analysis of rat brain tissue sections and sour orange (Citrus aurantium) leaves.

Influence of the interaction between nanoparticles and high brilliant laser radiation during μs-pulses on the ablation process of metals

A characteristic of the laser ablation process of metals with high brilliant radiation is a significant formation of nanoparticles within the vapour plume. Due to the interaction between the incoming radiation and the particles, the intensity is attenuated at the workpiece. This leads to a decrease of the ablation rate and the related ablation velocity. In order to verify the influence of the interaction between nanoparticles and high brilliant radiation on the ablation process, experimental and theoretical results of the laser ablation process of stainless steel with a single mode fiber laser are presented. For an ablation process with an intensity of 1.9×108W/cm², it is shown that the average particle size is 9nm. Within a further time-dependent analysis of the correlation between particle formation and ablation velocity, the beam of a test laser is directed through the vapour plume and the angle-dependent scattered radiation is detected. The results point out that a decrease of the ablation velocity corresponds with an increasing of the particle density within the ablation plume.

Aerosol formation and hydrogen co-deposition by colliding ablation plasma plumes of lithium and lead

In a high-repetition inertial fusion reactor, along with pellet implosions, the interior of target chamber is to be exposed to high-energy, short pulses of X-ray, unburned DT and He ash particles and pellet debris. As a result, wall materials will be subjected to ablation, ejecting particles in the plasma state to collide with each other in the center of volume. The interaction dynamics of ablation plasmas of lithium and lead, candidate first wall materials, has been investigated in the deposited energy density range from 3 to 10J/cm2/pulse at a repetition rate of 10Hz, each 6ns long. The plasma density and electron temperature of colliding ablation plumes have been found to vary from the order of 108–10131/cm3 and from 0.7 to 1.5eV, respectively. The formation of aerosol in the form of droplet has been observed with diameters between 100nm and 10μm. Also, hydrogen co-deposition has been found to occur particularly for colliding plumes of lithium, resulting in the H/Li atomic ratio from 0.15 to 0.27 in the hydrogen partial pressure range from 10 to 50Pa.

Time dynamics of burst-train filamentation assisted femtosecond laser machining in glasses

Bursts of femtosecond laser pulses with a repetition rate of f = 38.5MHz were created using a purpose-built optical resonator. Single Ti:Sapphire laser pulses, trapped inside a resonator and released into controllable burst profiles by computer generated trigger delays to a fast Pockels cell switch, drove filamentation-assisted laser machining of high aspect ratio holes deep into transparent glasses. The time dynamics of the hole formation and ablation plume physics on 2-ns to 400-ms time scales were examined in time-resolved side-view images recorded with an intensified-CCD camera during the laser machining process. Transient effects of photoluminescence and ablation plume emissions confirm the build-up of heat accumulation effects during the burst train, the formation of laser-generated filaments and plume-shielding effects inside the deeply etched vias. The small time interval between the pulses in the present burst train enabled a more gentle modification in the laser interaction volume that mitigated shock-induced microcracks compared with single pulses.

The effect of the target structure and composition on the ejection and transport of polymer molecules and carbon nanotubes in matrix-assisted pulsed laser evaporation

Matrix-assisted pulsed laser evaporation (MAPLE) is a prominent member of a broad and expanding class of laser-driven deposition techniques where a matrix of volatile molecules absorbs laser irradiation and provides the driving force for the ejection and transport of the material to be deposited. The mechanisms of MAPLE are investigated in coarse-grained molecular dynamic simulations focused on establishing the physical regimes and limits of the molecular transfer from targets with different structures and compositions. The systems considered in the simulations include dilute solutions of polymer molecules and individual carbon nanotubes (CNTs), as well as continuous networks of carbon nanotubes impregnated with solvent. The polymer molecules and nanotubes are found to be ejected only in the ablation regime and are incorporated into matrix-polymer droplets generated in the process of the explosive disintegration of the overheated matrix. The ejection and deposition of droplets explain the experimental observations of complex surface morphologies in films deposited by MAPLE. In simulations performed for MAPLE targets loaded with CNTs, the ejection of individual nanotubes, CNT bundles, and tangles with sizes comparable or even exceeding the laser penetration depth is observed. The ejected CNTs align along the flow direction in the matrix plume and tend to agglomerate into bundles at the initial stage of the ablation plume expansion. In a large-scale simulation performed for a target containing a network of interconnected CNT bundles, a large tangle of CNT bundles with the total mass of 50 MDa is separated from the continuous network and entrained with the matrix plume. No significant splitting and thinning of CNT bundles in the ejection process is observed in the simulations, suggesting that fragile structural elements or molecular agglomerates with complex secondary structures may be transferred and deposited to the substrate with the MAPLE technique.

Laser ablation and deposition of wide bandgap semiconductors: plasma and nanostructure of deposits diagnosis

Nanostructured CdS and ZnS films on Si (100) substrates were obtained by nanosecond pulsed laser deposition at the wavelengths of 266 and 532 nm. The effect of laser irradiation wavelength on the surface structure and crystallinity of deposits was characterized, together with the composition, expansion dynamics and thermodynamic parameters of the ablation plume. Deposits were analyzed by environmental scanning electron microscopy, atomic force microscopy and X-ray diffraction, while in situ monitoring of the plume was carried out with spectral, temporal and spatial resolution by optical emission spectroscopy. The deposits consist of 25–50 nm nanoparticle assembled films but ablation in the visible results in larger aggregates (150 nm) over imposed on the film surface. The aggregate free films grown at 266 nm on heated substrates are thicker than those grown at room temperature and in the former case they reveal a crystalline structure congruent with that of the initial target material. The observed trends are discussed in reference to the light absorption step, the plasma composition and the nucleation processes occurring on the substrate.

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.