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<i>In situ</i> structural kinetics of picosecond laser-induced heating and fragmentation of colloidal gold spheres
摘要： Fragmentation of colloidal 54 nm gold nanoparticles by picosecond laser pulses is recorded by time-resolved X-ray scattering, giving access to structural dynamics down to a 80 ps resolution. Lattice temperature and energy dissipation have been quantified to verify that the maximum applied fluence of 1800 J m?2 heats up the particles close to boiling. Already within 30 ns, particles with significantly lower particle sizes of 2 to 3 nm are detected, which hints towards an ultrafast process either by a thermal phase explosion or Coulomb instability. An arrested growth is observed on a microsecond time scale resulting in a final particle size of 3–4 nm with high yield. In this context, the fragmentation in a NaCl/NaOH solution seems to limit growth by electrostatic stabilization of fragments, whereas it does not modify the initial product sizes. The laser-induced fragmentation process is identified as a single-step, instantaneous reaction.
关键词： Coulomb instability,fragmentation,thermal phase explosion,time-resolved X-ray scattering,picosecond laser pulses,gold nanoparticles
更新于2025-09-23 15:21:01
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The effect of pulse duration on nanoparticle generation in pulsed laser ablation in liquids: Insights from large-scale atomistic simulations
摘要： 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) 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) 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.
关键词： phase explosion,pulsed laser ablation in liquids,molecular dynamics simulations,hydrodynamic instability,atomistic simulations,nanoparticles,nucleation and growth
更新于2025-09-19 17:13:59
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Laser Ablation - From Fundamentals to Applications || Nanosecond Laser Ablation: Mathematical Models, Computational Algorithms, Modeling
摘要： The basic mathematical models, computational algorithms, and results of mathematical modeling of various modes of laser action on metals are considered. It is shown that for mathematical description and analysis of the processes of laser heating, melting, and evaporation of condensed media, various theoretical approaches are used: continuum, kinetic, atomistic, etc. Each of them has its own field of applicability, its advantages, and disadvantages. Mathematical description of ns-laser ablation is usually carried out within the framework of continuum approach in the form of hydrodynamic models that take into account reaction of irradiated material to varying density, pressure, and energy both in the target and in the vapor-gas medium. Within the framework of continuum approach, a multiphase, multifront hydrodynamic model and computational algorithm were constructed that were designed for modeling ns-PLA of metal targets embedded in gaseous media. It is shown that proposed model and computational algorithm allow to carry out the simulation of interrelated mechanisms of heterogeneous and homogeneous evaporation of metals manifested as a series of explosive boiling. Modeling has shown that explosive boiling in metals occurs due to the presence of a near-surface temperature maximum. It has been established that in ns-PLA, exposure regimes can be realized in which a phase explosion is the main mechanism of material removal. The verification of reliability of obtained results was carried out by comparing experimental data and calculations with atomistic models.
关键词： explosive boiling,phase explosion,hydrodynamic model,laser action,nanosecond pulse,mathematical modeling,subsurface temperature maximum
更新于2025-09-12 10:27:22