Tatiana Itina

Material decomposition mechanisms in femtosecond laser interactions with metals

A numerical hydrodynamic study of femtosecond laser ablation is presented. A detailed analysis of material decomposition is performed using a thermodynamically complete equation of state with separate stable and metastable phase states and phase boundaries. The lifetime of the metastable liquid state is estimated based on the classical theory of homogeneous nucleation. In addition, mechanical fragmentation of the target material is controlled based on available criteria. As a result, several ablation mechanisms are observed. A major fraction of the ablated material, however, is found to originate from the metastable liquid region, which is decomposed either thermally in the vicinity of the critical point into a liquid-gas-mixture or mechanically at high strain rate and negative pressure into liquid droplets and chunks. The calculation results explain available experimental findings.

Comparative investigation of solar cell thin film processing using nanosecond and femtosecond lasers

The purpose of the present study was to examine the possibility of laser-machining of CuInSe2-based photovoltaic devices. Therefore, ablation thresholds and ablation rates of ZnO, CuInSe2 and Mo thin films have been measured for irradiation with nanosecond laser pulses of ultraviolet and visible light and subpicosecond laser pulses of a Ti : sapphire laser. The experimental results were compared with the theoretical evaluation of the samples heat regime obtained from numerical calculations. In addition, the photo-electrical properties of the solar cells were measured before and after laser-machining. Scanning electron microscopy and energy dispersive x-ray analyses were employed to characterize the laser-induced ablation channels. As a result, two phenomena were found to limit the laser-machining process: (i) residues of Mo that were projected onto the walls of the ablation channel and (ii) the metallization of the CuInSe2 semiconductor close to the channel. Both effects lead to a shunt in the device that decreases the photovoltaic efficiency. As a consequence of these limiting effects, micromachining of CuInSe2-based solar cells was not possible with nanosecond laser pulses. Only subpicosecond laser pulses provided selective or complete ablation of the thin layers without a relevant change in the photoelectrical properties.

MONTE CARLO SIMULATION OF PULSED LASER ABLATION FROM TWO-COMPONENT TARGET INTO DILUTED AMBIENT GAS

Laser ablation from a binary target into a diluted gas background is studied by means of a Monte Carlo simulation. The influence of the ambient gas on the spatial and mean energy distribution of particles deposited at the distant detector is considered. Thermalization of the particles, the random scattering effect and the backscattering of particles were observed. Considerable modification of the deposited film thickness profiles due to collisions of the ablated particles with the ambient gas is shown. The increase of the ambient gas pressure was found to affect the stoichiometry distribution of deposited and backscattered particles. The study is of a particular interest for the development of the thin film growing technique known as pulsed laser deposition.

Possible surface plasmon polariton excitation under femtosecond laser irradiation of silicon

The mechanisms of ripple formation on silicon surface by femtosecond laser pulses are investigated. We demonstrate the transient evolution of the density of the excited free-carriers. As a result, the experimental conditions required for the excitation of surface plasmon polaritons are revealed. The periods of the resulting structures are then investigated as a function of laser parameters, such as the angle of incidence, laser fluence, and polarization. The obtained dependencies provide a way of better control over the properties of the periodic structures induced by femtosecond laser on the surface of a semiconductor material.

Molecular dynamics simulations of matrix-assisted laser desorption—connections to experiment

The molecular dynamics (MD) simulation technique has been applied to investigate fundamental aspects of matrix-assisted laser desorption. In this paper, we focus on direct comparisons of the results from the simulations with experimental data and on establishing links between the measured or calculated parameters and the basic mechanisms of molecular ejection. The results on the fluence dependence of the ablation/desorption yields and composition of the ejected plume are compared with mass spectrometry and trapping plate experiments. Implications of the prediction of a fluence threshold for ablation are discussed. The strongly forward-peaked velocity and angular distributions of matrix and analyte molecules, predicted in the simulations, are related to the experimental distributions. The shapes and amplitudes of the acoustic waves transmitted from the absorption region through the irradiated sample are compared to recent photoacoustic measurements and related to the ejection mechanisms. The conformational changes during plume evolution and the ejection velocities of analyte molecules are studied and the directions for future investigations are discussed. Finally, we demonstrate that the MD simulation technique can be used to model other processes relevant to mass spectrometry applications, such as laser disintegration of aerosol particles and laser ablation in the presence of photochemical reactions.

Suppression of ablation in femtosecond double pulse experiments

We report the physical reasons of a curious decrease in the crater depth observed for long delays in experiments with two successive femtosecond pulses. Detailed hydrodynamic modeling demonstrates that the ablation mechanism is dumped when the delay between the pulses exceeds the electron-ion relaxation time. In this case, the interaction of the second laser pulse with the expanding target material leads to the formation of the second shock wave suppressing the rarefaction wave created by the first pulse. The evidence of this effect follows from the pressure and density profiles obtained at different delays after the first laser pulse.

Combined continuous–microscopic modeling of laser plume expansion

A hybrid model is developed to study the dynamics of laser plume expansion in vacuum or into a background gas. The method takes advantages of both continuous and microscopic simulation approaches. As a result of the combination of two different numerical methods, such as, large particles and direct Monte Carlo simulation, the model describes high-rate laser ablation for a wide range of background pressures (from zero to hundreds Pa). The model is used to investigate laser plume interaction with background gases. Particularly, the plume–gas mixing and energy exchange are taken into account. The dynamics of the laser plume expansion is investigated. Snowplow effect is observed at sufficiently high pressures. At smaller pressures, strong plume–gas mixing takes place near the contact surface. The simulation results explain experimentally obtained spatial maps of the reaction products formed during the plume expansion into a reactive background gas.

Numerical study of the role of a background gas and system geometry in pulsed laser deposition

The transport of laser ablated particles through a Maxwell-distributed ambient gas is simulated by Monte Carlo method. Three system geometry configurations frequently appearing in laser ablation experiments are considered: plume tilting, use of an interacting gas jet, and deposition on a substrate placed perpendicular to the laser-irradiated surface. The influence of the ambient gas on the formation of film thickness profiles and kinetic energy distributions of the deposited particles is studied. The thermalization of the laser plume and the backscattering of the ablated particles due to collisions with the background gas are investigated from two-dimensional film thickness distributions.

Monte Carlo simulation study of the effects of nonequilibrium chemical reactions during pulsed laser desorption

Monte Carlo simulation is used to study the role of chemical reactions in the gas flow of particles laser desorbed from the target into a vacuum. The influence of recombination and dissociation processes on the properties of the gas flow is considered. It was found that chemical reactions have a significant effect on the composition of the desorption jet and on the angular and mean energy distributions of the desorbed particles. The study of these phenomena is of a particular interest for the understanding of the process of thin film deposition by pulsed laser ablation.

Matrix-assisted pulsed laser evaporation of polymeric materials: a molecular dynamics study

Abstract Matrix-assisted pulsed laser evaporation (MAPLE) has been recently developed to deposit high-quality thin films for a wide range of polymeric materials. To analyze the evaporation of polymer molecules in MAPLE, we present a molecular dynamics (MD) simulation of laser ablation where the target material is modeled as a solution of polymer molecules in a molecular matrix. The breathing sphere model is used for MD simulations of laser ablation of the molecular matrix. Polymer molecules are described using a bead-spring model, where each bead represents one or several polymer groups. The initial stage of polymer ejection is investigated at different laser fluences and pulse durations. The influence of polymer molecules on the stability of clusters formed in the plume and the processes that can lead to polymer decomposition are discussed.