In pulsed laser deposition, thin film growth is mediated by a laser-generated plasma, whose properties are critical for controlling the film microstructure. The advent of 2D materials has renewed the interest in how this ablation plasma can be used to manipulate the growth and processing of atomically thin systems. For such purpose, a quantitative understanding of the density, charge state, and kinetic energy of plasma constituents is needed at the location where they contribute to materials processes. Here we study laser-induced plasmas over expansion distances of several centimeters from the ablation target, which is the relevant length scale for materials growth and modification. The study is enabled by a fast implementation of a laser ablation/plasma expansion model using an adaptive Cartesian mesh solver. Simulation outcomes for KrF excimer laser ablation of Cu are compared with Langmuir probe and optical emission spectroscopy measurements. Simulation predictions for the plasma-shielding threshold, the ionization state of species in the plasma, and the kinetic energy of ions, are in good correspondence with experimental data. For laser fluences of 1-4 J/cm 2 , the plume is dominated by Cu 0 , with small concentrations of Cu + and electrons at the expansion front. Higher laser fluences (e.g., 7 J/cm 2 ) lead to a Cu + -rich plasma, with a fully ionized leading edge where Cu 2+ is the dominant species. In both regimes, simulations indicate the presence of a low-density, high-temperature plasma expansion front with a high degree of ionization that may play a significant role in doping, annealing, and kineticallydriven phase transformations in 2D materials.
We carry out simulations of laser plasmas generated during UV nanosecond pulsed laser ablation of the chalcogens selenium (Se) and tellurium (Te), and compare the results to experiments. We take advantage of a 2D-axisymmetric, adaptive Cartesian mesh framework that enables plume simulations out to centimeter distances over tens of microseconds. Our model and computational technique enable comparison to laser-plasma applications where the long-term behavior of the plume is of primary interest, such as pulsed laser synthesis and modification of materials. An effective plasma absorption term is introduced in the model, allowing the simulation to be constrained by experimental time-of-flight kinetic energy distributions. We show that the effective simulation qualitatively captures the key characteristics of the observed laser plasma, including the effect of laser spot size. Predictions of full-scale experimentally-constrained Se and Te plasmas for 4.0 J cm −2 laser fluence and 1.8 mm 2 circular laser spot area show distinct behavior compared to more commonly studied copper (Cu) plumes. The chalcogen plumes have spatial gradients of plasma density that are steeper than those for Cu by up to three orders of magnitude. Their spatial ion distributions have central bulges, in contrast to the edge-only ionization of Cu. For the irradiation conditions explored, the range of plasma temperatures for Se and Te is predicted to be higher than for Cu by more than 0.50 eV.
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