Nanoparticle Formation by Laser Ablation and by Spark Discharges — Properties, Mechanisms, and Control Possibilities

Laser ablation (LA) and spark discharge (SD) techniques are commonly used for nanoparticle (NP) formation. The produced NPs have found numerous applications in such areas as electronics, biomedicine, textile production, etc. Previous studies provide us information about the amount of NPs, their size distribution, and possible applications. On one hand, the main advantage of the LA method is in the possibilities of changing laser parameters and background conditions and to ablate materials with complicated stoichiometry. On the other hand, the major advantage of the SD technique is in the possibility of using several facilities in parallel to increase the yield of nanoparticles. To optimize these processes, we consider different stages involved and analyze the resulting plasma and nanoparticle (NP) parameters. Based on the performed calculations, we analyze nanoparticle properties, such as mean size and mean density. The performed analysis (shows how the experimental conditions are connected with the resulted nanoparticle characteristics in agreement with several previous experiments. Cylindrical plasma column expansion and return are shown to govern primary nanoparticle formation in spark discharge, whereas hemispherical shock describes quite well this process for nanosecond laser ablation at atmospheric pressure. In addition, spark discharge leads to the oscillations in plasma properties, whereas monotonous behavior is characteristic for nanosecond laser ablation. Despite the difference in plasma density and time evolutions calculated for both phenomena, after well-defined delays, similar critical nuclei have been shown to be formed by both techniques. This result is attributed to the fact that whereas larger evaporation rate is typical for nanosecond laser ablation, a mixture of vapor and background gas determines the supersaturation in the case of spark

Rippled area formed by surface plasmon polaritons upon femtosecond laser double-pulse irradiation of silicon: the role of carrier generation and relaxation processes

The formation of laser-induced periodic surface structures (LIPSS, ripples) upon irradiation of silicon with multiple irradiation sequences consisting of femtosecond laser pulse pairs (pulse duration 150 fs, central wavelength 800 nm) is studied numerically using a rate equation system along with a two-temperature model accounting for one- and two-photon absorption and subsequent carrier diffusion and Auger recombination processes. The temporal delay between the individual equal-energy fs-laser pulses was varied between $0$ and $\sim 4$ ps for quantification of the transient carrier densities in the conduction band of the laser-excited silicon. The results of the numerical analysis reveal the importance of carrier generation and relaxation processes in fs-LIPSS formation on silicon and quantitatively explain the two time constants of the delay dependent decrease of the Low-Spatial-Frequency LIPSS (LSFL) area observed experimentally. The role of carrier generation, diffusion and recombination are quantified individually.Comment: 5 pages, 5 figures, Conference On Laser Ablation (COLA) 2013. The final publication is available at http://link.springer.com. Accepted for publication in Applied Physics

Thermoplastic deformation of silicon surfaces induced by ultrashort pulsed lasers in submelting conditions

A hybrid 2D theoretical model is presented to describe thermoplastic deformation effects on silicon surfaces induced by single and multiple ultrashort pulsed laser irradiation in submelting conditions. An approximation of the Boltzmann transport equation is adopted to describe the laser irradiation process. The evolution of the induced deformation field is described initially by adopting the differential equations of dynamic thermoelasticity while the onset of plastic yielding is described by the von Mise's stress. Details of the resulting picometre sized crater, produced by irradiation with a single pulse, are then discussed as a function of the imposed conditions and thresholds for the onset of plasticity are computed. Irradiation with multiple pulses leads to ripple formation of nanometre size that originates from the interference of the incident and a surface scattered wave. It is suggested that ultrafast laser induced surface modification in semiconductors is feasible in submelting conditions, and it may act as a precursor of the incubation effects observed at multiple pulse irradiation of materials surfaces.Comment: To appear in the Journal of Applied Physic

From random inhomogeneities to periodic nanostructures induced in bulk silica by ultrashort laser

International audienceFemtosecond laser-induced volume nanograting formation is numerically investigated. The developed model solves nonlinear Maxwell's equations coupled with multiple rate free carrier density equations in the presence of randomly distributed inhomogeneities in fused silica. As a result of the performed calculations, conduction band electron density is shown to form nanoplanes elongated perpendicular to the laser polarization. Two types of nanoplanes are identified. The structures of the first type have a characteristic period of the laser wavelength in glass and are attributed to the interference of the incident and the inhomogeneity-scattered light waves. Field components induced by coherent multiple scattering in directions perpendicular to the laser polarization are shown to be responsible for the formation of the second type of structures with a subwavelength periodicity. In this case, the influence of the inhomogeneity concentration on the period of nanoplanes is shown. The calculation results not only help to identify the physical origin of the self-organized nanogratings, but also explain their period and orientation

Femtosecond laser irradiation of dielectric materials containing randomly-arranged nanoparticles

International audienceWe investigate femtosecond laser irradiation of dielectric materials containing randomly-arranged nanoparticles. For this, numerical modeling is performed based on three different methods: Mie theory, static solution of linear Maxwell's equations and a solution of nonlinear Maxwell's equations together with kinetic equations for free electron excitation/relaxation processes. First two approaches are used to define the static intensity distribution and to analyze the electromagnetic interaction between the nanoparticles. The third method allows us to investigate the complex dynamics of the laser-matter interaction. Multiphoton absorption is shown to be responsible for electron plasma generation in the regions of strong intensity enhancements in the vicinity of nanoparticles. The irradiation of the dielectric material leads to the elongation of nanoplasmas by the near-field enhancement perpendicular to the laser polarization and to their strong interaction resulting in periodic arrangement. Numerical results shed light on such effects as femtosecond laser-induced nanograting formation

Analyses of femtosecond laser ablation of Ti, Zr, Hf

Femtosecond laser ablation of Ti, Zr and Hf has been investigated by means of in-situ plasma diagnostics. Fast plasma imaging with the aid of an intensified charged coupled device (ICCD) camera was used to characterise the plasma plume expansion on a nanosecond time scale. Time- and spaceresolved optical emission spectroscopy was employed to perform time-of-flight measurements of ions and neutral atoms. It is shown that two plasma components with different expansion velocities are generated by the ultra-short laser ablation process. The expansion behaviour of these two components has been analysed as a function of laser fluence and target material. The results are discussed in terms of mechanisms responsible for ultra-short laser ablation