Atomistic modeling of pulsed laser ablation in liquid: spatially and time-resolved maps of transient nonequilibrium states and channels of nanoparticle formation

Chen, Chaobo; Zhigilei, Leonid V.

doi:10.1007/s00339-023-06525-0

Cited by 9 publications

(5 citation statements)

References 93 publications

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“…The highest power-specific productivity achieved in these experiments was 12.8 mg/(h W) (equivalent to 3.55 μg/J) for the LFL of IrO 2 -MP (1) which is already comparable to the highest reported power-specific productivity for the laser ablation of platinum in water (37.8 mg/(h W) or 10.5 μg/J) when using a high power laser-based nanoparticle synthesis setup . Recently, detailed computational studies on FeNi LAL in different fluence regimes predicted ablation energy efficiency reaching the maximum level of slightly above 7 μg/J . While the conventional NP-LFL is even limited to 0.32 mg/(h W) (or 0.09 μg/J) to minimize the growth of the produced nanoparticles, this shows great potential of MP-LFL for energy-efficient synthesis of ultrasmall ligand-free NPs.…”

Section: Results and Discussionsupporting

confidence: 56%

“…9 Recently, detailed computational studies on FeNi LAL in different fluence regimes predicted ablation energy efficiency reaching the maximum level of slightly above 7 μg/J. 44 While the conventional NP-LFL is even limited to 0.32 mg/(h W) (or 0.09 μg/J) to minimize the growth of the produced nanoparticles, 45 this shows great potential of MP-LFL for energy-efficient synthesis of ultrasmall ligand-free NPs. Regarding the present downsizing mechanism, earlier studies discussed both, the photothermal and shock-wave-induced nanoparticle generation.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Continuous and Scalable Laser Synthesis of Atom Clusters with Tunable Surface Oxidation for Electrocatalytic Water Splitting

Tack,

Usama,

Kazamer

et al. 2024

ACS Appl. Energy Mater.

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The laser-based synthesis of colloidal nanoparticles consists of several established methods to produce high-purity, active, and durable metal and oxide catalysts. Among them, only laser fragmentation in a liquid jet produces monodisperse, sub-5 nm nanoparticles in a fully continuous operation. However, the nanoparticle yield and laser power-specific productivity are still below the established gram-scale laser ablation method. In addition, little is known about how the initial particle size, oxidation, and the number of laser pulses affect the generated particle size and oxidation state, especially when using commercial microparticles. In this work, we address these shortcomings with the example of iridium as an important benchmark catalyst for the acidic oxygen evolution reaction. Starting from iridium microparticles, a significant improvement in the laser power-specific productivity of nanoparticles was observed when the initial particle concentrations were increased to several grams per liter. The number of applied laser pulses controls the degree of nanoparticles' surface oxidation, as shown by XPS measurements and DFT calculations, while the monodisperse ∼2 nm product particle diameter was unaffected by the initial particle size and concentration, highlighting the process robustness. Additionally, the particles exhibit a benchmark level of catalytic activity with the lowest overpotential of 0.33 V vs RHE @ 10 mA/cm 2 . To summarize, the continuous laser fragmentation of microparticles in water has great potential in the green synthesis of ultrasmall catalysts.

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Section: Results and Discussionsupporting

confidence: 56%

Section: ■ Results and Discussionmentioning

confidence: 99%

Continuous and Scalable Laser Synthesis of Atom Clusters with Tunable Surface Oxidation for Electrocatalytic Water Splitting

Tack,

Usama,

Kazamer

et al. 2024

ACS Appl. Energy Mater.

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“…Both the representative TEM image in Figure a and the high-resolution image in Figure 2b of the Supporting Information show that mostly spherical Au NPs were gained by the laser synthesis. Given previous theoretical predictions, ,, the spherical NPs from laser ablation in liquids are likely to be enriched with internal planar defects. Consequently, the laser-generated nanoparticles, despite their polydispersity, were included to determine how sensitive our study concept (joining theory and experiment) and the synthesis procedure (LFL) are to the initial particle size distribution, which is characteristic for the laser synthesis.…”

Section: Methodsmentioning

confidence: 76%

Physical Regimes and Mechanisms of Picosecond Laser Fragmentation of Gold Nanoparticles in Water from X-ray Probing and Atomistic Simulations

Plech,

Tack,

Huang

et al. 2024

ACS Nano

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Laser fragmentation in liquids has emerged as a promising green chemistry technique for changing the size, shape, structure, and phase composition of colloidal nanoparticles, thus tuning their properties to the needs of practical applications. The advancement of this technique requires a solid understanding of the mechanisms of laser−nanoparticle interactions that lead to the fragmentation. While theoretical studies have made impressive practical and mechanistic predictions, their experimental validation is required. Hence, using the picosecond laser fragmentation of Au nanoparticles in water as a model system, the transient melting and fragmentation processes are investigated with a combination of timeresolved X-ray probing and atomistic simulations. The direct comparison of the diffraction profiles predicted in the simulations and measured in experiments has revealed a sequence of several nonequilibrium processes triggered by the laser irradiation. At low laser fluences, in the regime of nanoparticle melting and resolidification, the results provide evidence of a transient superheating of crystalline nanoparticles above the melting temperature. At fluences about three times the melting threshold, the fragmentation starts with evaporation of Au atoms and their condensation into small satellite nanoparticles. As fluence increases above five times the melting threshold, a transition to a rapid (explosive) phase decomposition of superheated nanoparticles into small liquid droplets and vapor phase atoms is observed. The transition to the phase explosion fragmentation regime is signified by prominent changes in the small-angle X-ray scattering profiles measured in experiments and calculated in simulations. The good match between the experimental and computational diffraction profiles gives credence to the physical picture of the cascade of thermal fragmentation regimes revealed in the simulations and demonstrates the high promise of the joint tightly integrated computational and experimental efforts.

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“…Once the plasma plume collapses and the cavitation bubble is formed from the evaporation of the surrounding liquid, the ions and atoms of the bulk target are released to the liquid media due to the rapid release of vapor, [ 3 ] while larger droplets are ejected through the photomechanical spallation. [ 4 ] The process is followed by the condensation due to the rapid quenching by the liquid (evaporation–condensation mechanism [ 5 ] ). Subsequently, primary NPs are formed in the liquid media through condensation nucleation, [ 6 ] while coalescence and growth contribute to the formation of larger secondary particle.…”

Section: Introductionmentioning

confidence: 99%

Parallel Diffractive Multi‐Beam Pulsed‐Laser Ablation in Liquids Toward Cost‐Effective Gram Per Hour Nanoparticle Productivity

Khairani,

Spellauge,

Riahi

et al. 2024

Advanced Photonics Research

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Nanoparticles (NPs) generated by pulsed‐laser ablation in liquids (PLAL) have benefited many key applications due to their versatility, enlarged surface area, and high purity. However, scaling up NPs production represents one of the main requisites to commercialize this technology. The established upscaling strategy demands high power and repetition rate laser source with fast scanning systems, which are not widely available and costly. Herein, a cost‐effective alternative is proposed, the addition of static diffractive optical elements to achieve parallel processing through the multi‐beam PLAL (MB‐PLAL). In MB‐PLAL, the optimum repetition rate is reduced to compensate laser energy splitting, hence achieving a higher interpulse distance, reducing pulse shielding, and increasing NPs productivity. MB‐PLAL with 11 beams reached a factor 4 productivity increase for iron–nickel alloy (Fe50Ni50) NPs compared to the single‐beam setup (0.4–1.6 g h−1), and a factor 3 increase for gold (Au) NPs (0.32–0.94 g h−1). The scalability of the proposed MB‐PLAL technique setup is confirmed by Au and Fe50Ni50 NPs productivity experiments using 1, 6, and 11 beams, showing a linear increase in productivity.

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Atomistic modeling of pulsed laser ablation in liquid: spatially and time-resolved maps of transient nonequilibrium states and channels of nanoparticle formation

Cited by 9 publications

References 93 publications

Continuous and Scalable Laser Synthesis of Atom Clusters with Tunable Surface Oxidation for Electrocatalytic Water Splitting

Continuous and Scalable Laser Synthesis of Atom Clusters with Tunable Surface Oxidation for Electrocatalytic Water Splitting

Physical Regimes and Mechanisms of Picosecond Laser Fragmentation of Gold Nanoparticles in Water from X-ray Probing and Atomistic Simulations

Parallel Diffractive Multi‐Beam Pulsed‐Laser Ablation in Liquids Toward Cost‐Effective Gram Per Hour Nanoparticle Productivity

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