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The generation of colloidal solutions of chemically clean nanoparticles through pulsed laser ablation in liquids (PLAL) has evolved into a thriving research field that impacts industrial applications. The complexity and multiscale nature of PLAL make it difficult to untangle the various processes involved in the generation of nanoparticles and establish the dependence of nanoparticle yield and size distribution on the irradiation parameters. Large-scale atomistic simulations have yielded important insights into the fundamental mechanisms of ultrashort (femtoseconds to tens of picoseconds) PLAL and provided a plausible explanation of the origin of the experimentally observed bimodal nanoparticle size distributions. In this paper, we extend the atomistic simulations to short (hundreds of picoseconds to nanoseconds) laser pulses and focus our attention on the effect of the pulse duration on the mechanisms responsible for the generation of nanoparticles at the initial dynamic stage of laser ablation. Three distinct nanoparticle generation mechanisms operating at different stages of the ablation process and in different parts of the emerging cavitation bubble are identified in the simulations. These mechanisms are (1) the formation of a thin transient metal layer at the interface between the ablation plume and water environment followed by its decomposition into large molten nanoparticles, (2) the nucleation, growth, and rapid cooling/solidification of small nanoparticles at the very front of the emerging cavitation bubble, above the transient interfacial metal layer, and (3) the spinodal decomposition of a part of the ablation plume located below the transient interfacial layer, leading to the formation of a large population of nanoparticles growing in a high-temperature environment through inter-particle collisions and coalescence. The coexistence of the three distinct mechanisms of the nanoparticle formation at the initial stage of the ablation process can be related to the broad nanoparticle size distributions commonly observed in nanosecond PLAL experiments. The strong dependence of the nanoparticle cooling and solidification rates on the location within the low-density metal–water mixing region has important implications for the long-term evolution of the nanoparticle size distribution, as well as for the ability to quench the nanoparticle growth or dope them by adding surface-active agents or doping elements to the liquid environment.
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Modeling for Chemical-Etching Enhanced Pulsed Laser Ablation
Pulsed laser ablation (PLA) under active liquid confinement, also known as chemical etching enhanced pulsed laser ablation (CE-PLA), has emerged as a novel laser processing methodology, which breaks the current major limitation in underwater PLA caused by the breakdown plasma and effectively improves the efficiencies of underwater PLA-based processes, such as laser-assisted nano-/micro-machining and laser shock processing. Despite of experimental efforts, little attention has been paid on CE-PLA process modeling. In this study, an extended two-temperature model is proposed to predict the temporal/spatial evolution of the electron-lattice temperature and the ablation rate in the CE-PLA process. The model is developed with considerations on the temperature-dependent electronic thermal properties and optical properties of the target material. The ablation rate is formulated by incorporating the mutual promotion between ablation and etching processes. The simulation results are validated by the experimental data of CE-PLA of zinc under the liquid confinement of hydrogen peroxide.
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- Award ID(s):
- 1825739
- PAR ID:
- 10379359
- Date Published:
- Journal Name:
- Proceedings of the ASME 2019 14th International Manufacturing Science and Engineering Conference
- Volume:
- 1
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Conference Paper:
- https://doi.org/10.1115/MSEC2019-2844
