Abstract
The mechanisms of picosecond pulse laser ablation in liquid are investigated in a series of large-scale atomistic simulations performed for FeNi targets irradiated in a liquid environment by picosecond laser pulses at a broad range of fluences. The simulations reveal the existence of three fluence regimes featuring different dominant mechanisms of material ejection and nanoparticle formation. These are (1) the low fluence regime, where atomic clusters and small nanoparticles form through the evaporation of metal atoms followed by condensation in a low-density region at the front of the ablation plume, (2) the medium fluence regime, where roughening and decomposition of a top part of a transient spongy structure of interconnected liquid regions leads to the formation of large nanoparticles, and (3) the high fluence regime, where the nanoparticles form primarily at the phase separation front propagating through the ablation plume cooled from the supercritical state by expansion against the liquid environment and mixing with the liquid. The generation of the largest nanoparticles is observed in the medium fluence regime, and both the maximum size of the nanoparticles and the energy efficiency of the material conversion into nanoparticles decrease upon transition to the high fluence regime. Some of the nanoparticles experience extreme quench rates and rapidly solidify under conditions of deep undercooling, yielding a population of defect-rich nanoparticles of interest for practical applications. The results of the simulations are mapped to the conditions realized within a laser spot irradiated by a beam with a Gaussian spatial profile, where different ablation regimes are activated simultaneously in different parts of the laser spot. The spatially and time-resolved maps of the transient nonequilibrium states predicted in the simulations provide a comprehensive picture of the ablation dynamics and a solid foundation for interpretation of the results of time-resolved experimental probing of the initial stage of the ablation process.
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Acknowledgements
Financial support for this work was provided by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under contract number DE-SC0019191, as well as the National Science Foundation (NSF) through grants CMMI-1663429 and CBET-2126785. Leonid V. Zhigilei also acknowledges the Research Award of the Alexander von Humboldt Foundation. Computational support was provided by the NSF through the Extreme Science and Engineering Discovery Environment (Grant No. TGDMR110090).
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Chen, C., Zhigilei, L.V. Atomistic modeling of pulsed laser ablation in liquid: spatially and time-resolved maps of transient nonequilibrium states and channels of nanoparticle formation. Appl. Phys. A 129, 288 (2023). https://doi.org/10.1007/s00339-023-06525-0
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DOI: https://doi.org/10.1007/s00339-023-06525-0