Nanoparticles size modifications during femtosecond laser ablation of nickel in vacuum

Nanoparticles were synthesized by irradiating a nickel target with femtosecond laser pulses in high vacuum, and subsequently analyzed. The proof-of-principle experiments aim to modify the size characteristics of the produced nanoparticles. For nickel it is found that: (i) ultraviolet laser pulses lead to a remarkable change in the nanoparticles size distribution with respect to visible laser pulses; (ii) irradiation of the femtosecond pulses induced ablation plume with a second, delayed ultraviolet laser pulse can change the size characteristics of the produced nanoparticles.     

Experimental investigation of ablation efficiency and plasma expansion during femtosecond and nanosecond laser ablation of silicon

Femtosecond laser (Ti:sapphire, 100 fs pulse duration) ablation of silicon in air was compared with nanosecond laser (Nd:YAG, 3 ns pulse duration) ablation at ultraviolet wavelength (266 nm). Laser ablation efficiency was studied by measuring crater depth as a function of pulse number. For the same number of laser pulses, the fs-ablated crater was about two times deeper than the ns-crater. The temperature and electron number density of the laser-induced plasma were determined from spectroscopic measurements. The electron number density and temperature of fs-induced plasmas decreased faster than ns-induced plasmas due to different energy deposition mechanisms. Images of the laser-induced plasma were obtained with femtosecond time-resolved laser shadowgraph imaging. Plasma expansion in both the perpendicular and the lateral directions were compared. PACS 52.38.Mf; 52.30.-q     

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.     

Time evolution of the infrared laser ablation plasma plume of SiO

The spatio-temporal evolution of the silicon monoxide SiO plasma produced by a high-power CO₂ pulsed laser has been investigated using optical emission spectroscopy (OES) and imaging methods. The formed plasma was found to be strongly ionized, yielding Si⁺, O⁺, Si²⁺, O²⁺ and Si³⁺ species, rich in neutral silicon and oxygen atoms, and very weak molecular bands of SiO time-integrated and time-resolved two-dimensional OES plasma profiles were recorded as a function of emitted wavelength and distance from the target. The temporal behavior of specific emission lines of Si, Si⁺, O⁺, Si²⁺ and O²⁺ was characterized. The results show a faster decay of O²⁺ and Si²⁺ than that of O⁺, Si⁺ and Si. The Stark broadening of isolated single-ionized silicon emission lines was employed for deducing the electron density during the plasma expansion. The relative intensities of two Si²⁺ lines were used to calculate the time evolution of the plasma temperature.     

Experimental investigation of recoil-momentum-generation efficiency under near-IR femtosecond laser ablation of refractory metals in vacuum

The use of ultrashort laser pulses is a way to increase recoil momentum under laser ablation of materials, because, in this case, the energy deposition per unit volume of the target material is substantially higher due to reduced heat dissipation. By using methods of combined interferometry, we estimated the specific impulse (～200–900 s), momentum coupling coefficient (～2 × 10^?5?3 × 10^?4 Ns/J), laser-energy conversion efficiency to kinetic energy of the gas-plasma flow (～0.05–0.82), and degree of the gas-plasma flow monochromaticity (～0.72–0.92) under femtosecond (τ ～ 45 fs, λ ～ 800 nm) ablation of refractory metals (Ti, Zr, Mo, and Nb) in vacuum.     

Thermodynamic evolution of materials during laser ablation under pico and femtosecond pulses

Using molecular-dynamics, we study the thermodynamic evolution of a simple two-dimensional Lennard–Jones system during laser ablation for pulse durations ranging from 200 fs to 400 ps. We briefly review results previously obtained for fs pulses where the evolution of the material was shown to be solely a function of the locally absorbed energy (provided that only thermal effects are important), i.e., is adiabatic. For longer pulses (100 and 400 ps) the situation becomes more complex, as the relaxation path also depends on the position in the target and on the timescale on which expansion occurs. We show that, in contrast to fs pulses, the material ejected following ps laser irradiation does not enter the liquid–vapor metastable region before ablation occurs, hence showing that phase explosion is not the dominant mechanism in this regime. Following on from previous work, we propose that trivial fragmentation is the main ablation mechanism. PACS 79.20.Ds; 79.20.Ap; 61.80.Az     

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.     

Time-resolved plasma diagnostics and mass removal during single-pulse laser ablation

Laser ablation processes occurring over several orders of magnitude in time were investigated by using time-resolved spectroscopy, shadowgraphs and interferograms. A picosecond ablation plasma was measured with an electron density on the order of 10²⁰ cm^-3 originating from the breakdown of air. The longitudinal expansion of this plasma was suppressed due to the development of a strong space-charge field. At post-pulse times, the lateral (radial) expansion of the plasma was found to follow the relation, r~t^1/2, consistent with the expansion from an instantaneous line source of energy. The electron number density and temperature were deduced by measuring spectroscopic emission-line broadening during the early phase (30-300 ns) of a mass (atomic/ionic) plasma. These properties were measured as a function of the delay time and irradiance. Possible mechanisms such as inverse bremsstrahlung and self-regulation were used to describe the data before an explosion threshold of 20 GW/cm². The laser self-focusing and critical temperature are discussed to explain dramatic changes in these properties after the irradiance threshold. On the microsecond time scale, the surface explodes and large (>7m) particles are ejected. Mass removed from single-crystal silicon by high power (10⁹-10¹¹ W/cm²) single-pulse laser ablation is studied by measuring the crater morphology. Time-resolved shadowgraph images show that the rapid increase in the crater depth at the threshold corresponds to large-size droplets leaving the surface. This rapid growth of the crater volume is attributed to explosive boiling.     

Adaptive control of femtosecond laser ablation plasma emission

The influence of temporal pulse shaping on plasma plume generated by ultrafast laser irradiation of aluminum is investigated. Time resolved plasma emission spectroscopy is coupled with a temporal shaping procedure in a closed loop. The ionic emission is enhanced relative to the neutral one via an adaptive optimization strategy. The plasma emission efficiency in case of optimized and ultrashort temporal shapes of the laser pulses are compared, evidencing an enhancement of the ionization degree of the plasma plume. Simplified temporal shapes of the femtosecond laser pulses are extracted from the optimized shape and their corresponding effect on laser induced plasma emission is discussed.     

Energy efficiency of femtosecond laser ablation of refractory metals

We present the results of an experimental study of the ablation energy thresholds and ablated mass for a number of refractory metals (Ti, Zr, Nb, Mo) by femtosecond (τ _0.5 = 45–70 fs) exposed to laser pulses in the ultraviolet — near infrared range (λ = 266, 400, 800 nm) under atmospheric conditions and under vacuum (p ~ 10^–2 Pa). We have analyzed the ablation efficiency (mass yield per unit energy of the acting coherent radiation) and ablation energy thresholds vs. the laser pulse duration and photon energy.     

Energy efficiency of femtosecond laser ablation of polymer materials

We present the results of an experimental study of the ablation spectral energy thresholds for a number of polymer materials ((C₂F₄) _n , (CH₂O) _n ) exposed to femtosecond (τ_0.5 ~ 45–70 fs) laser pulses (λ ~ 266, 400, 800 nm) under atmospheric conditions and under vacuum (p ~ 10–2 Pa). We have analyzed the energy thresholds and the efficiency of optical, thermophysical, and gasdynamic processes in laser ablation vs. the laser pulse duration and photon energy.     

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.     

Probe studies of laser erosion plume arising at silicon ablation in vacuum

An erosion plume arising at the ablation of silicon by a solid-state laser (λ = 1.06 μm) is studied with a Langmuir probe. The time-of-flight curves of the probe ion current are obtained for a plasma beam formed by intersecting plumes from two targets and for an erosion plume from one silicon target. The probe-target distance is varied in the range 40–157 mm. The time-of-flight curves for the ions of the erosion plume are sums of the velocity one-dimensional Maxwell distributions for four groups of ions. It is found that a plasma beam formed by intersecting plumes from two targets does not contain all groups of ions present in initial plumes.     

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.     

Hydrodynamic modeling of femtosecond laser ablation of metals in vacuum and in liquid

We numerically examine the mechanisms involved in nanoparticle formation by laser ablation of metallic targets in vacuum and in liquid. We consider the very early ablation stage providing initial conditions for much longer plume expansion processes. In the case of ultrashort laser ablation, the initial population of primary nanoparticles is formed at this stage. When a liquid is present, the dynamics of the laser plume expansion differs from that in vacuum. Low compressibility of the ambient liquid results in strong confinement conditions. As a result, ablation threshold rises drastically, the ablated material is compressed, part of it becomes supersaturated and the backscattered material additionally heats the target. The extension of a molten layer leads to the additional ablation at a later stage also favoring nanoparticle formation. The obtained results thus explain recent experimental findings and help to predict the role of the experimental parameters. The performed analysis indicates ways of a control over nanoparticle synthesis.     

Study of the plasma plume generated during near IR femtosecond laser irradiation of silicon targets

Ti:sapphire femtosecond laser ablation of silicon has been investigated by Langmuir probe and time-gated optical emission spectroscopy. The measured spectra show the presence of a fast ion population preceding the main plume core of slow ions and neutrals produced by a thermal ablation mechanism. By analyzing the fluence thresholds for the emission of the two ion populations, we provide clear experimental evidence that fast ions are ejected non-thermally from the sample surface as a result of the Si surface supercritical state induced by the intense ultrashort laser pulse irradiation. PACS 52.50.Jm; 52.38.Mf; 79.20.Ds; 61.82.Fh     

Early stage of the material removal during ArF laser ablation of graphite

Material removal during ArF excimer laser ablation of graphite at atmospheric pressure was investigated by two independent methods; 1) by observation of the propagating properties of the shock wave generated by the carbonaceous ejecta and 2) by in situ measurement of the size distribution of carbon nanoparticles condensing in the ablation plume. This latter was carried out by a scanning mobility particle sizer system based on a differential mobility analyser. The performed measurements indicate that the material removal during ArF laser ablation consists of two steps at fluences above the threshold fluence. First, a thin layer of carbon (of the order of 1 nm) is removed by a quick desorption process, leading to shockwave formation. This process takes place in a ns time scale, and desorption rate estimations reveal that this can not be explained by thermal surface evaporation. Since to our knowledge there is no thermal process that could account for the estimated desorption rate, it is argued that this is a fast photochemical (i.e. non-thermal) process. The size distribution of the condensed nanoparticles related to this step shows a rising edge at diameters below 10 nm. At fluences above the ablation threshold, the majority of the material is ejected in the second phase, resulting in condensation of carbon nanoparticles, peaking at 50 nm diameters in the size spectrum. Both shockwave formation and material removal are also detected well below the ablation threshold fluence, which is attributed to the photochemical process. PACS 61.46.+w; 81.16.Mk