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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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Multiscale modeling of short pulse laser induced amorphization of silicon
Silicon surface amorphization by short pulse laser irradiation is a phenomenon of high importance for device manufacturing and surface functionalization. To provide insights into the processes responsible for laser-induced amorphization, a multiscale computational study combining atomistic molecular dynamics simulations of nonequilibrium phase transformations with continuum-level modeling of laser-induced melting and resolidification is performed. Atomistic modeling provides the temperature dependence of the melting/solidification front velocity, predicts the conditions for the transformation of the undercooled liquid to the amorphous state, and enables the parametrization of the continuum model. Continuum modeling, performed for laser pulse durations from 30 ps to 1.5 ns, beam diameters from 5 to 70 μm, and wavelengths of 532, 355, and 1064 nm, reveals the existence of two threshold fluences for the generation and disappearance of an amorphous surface region, with the kinetically stable amorphous phase generated at fluences between the lower and upper thresholds. The existence of the two threshold fluences defines the spatial distribution of the amorphous phase within the laser spot irradiated by a pulse with a Gaussian spatial profile. Depending on the irradiation conditions, the formation of a central amorphous spot, an amorphous ring pattern, and the complete recovery of the crystalline structure are predicted in the simulations. The decrease in the pulse duration or spot diameter leads to an accelerated cooling at the crystal–liquid interface and contributes to the broadening of the range of fluences that produce the amorphous region at the center of the laser spot. The dependence of the amorphization conditions on laser fluence, pulse duration, wavelength, and spot diameter, revealed in the simulations, provides guidance for the development of new applications based on controlled, spatially resolved amorphization of the silicon surface.
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- PAR ID:
- 10576859
- Publisher / Repository:
- AIP Publishing
- Date Published:
- Journal Name:
- Journal of Applied Physics
- Volume:
- 136
- Issue:
- 21
- ISSN:
- 0021-8979
- Page Range / eLocation ID:
- 213103
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1063/5.0240532
