skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Experimental and computational investigation into the hydrodynamics and chemical dynamics of laser ablation aluminum plasmas
Laser ablation plasma chemistry is governed by a complex interplay between hydrodynamic plasma-gas mixing processes, thermodynamics, and rapid high-temperature chemical reactions. In this work, we investigate the gas-phase oxidation chemistry of ns-laser ablation aluminum plasmas in air using optical spectroscopy combined with advanced multi-physics modeling. Experimental measurements demonstrate the formation of AlO in the plasma plume as early as 1 μs while computational results reveal that several Al x O y species are distributed in the periphery of the plume at even earlier times (<20 ns) in the presence of large temperature gradients and strong shockwaves. Interactions with the ablation crater during rapid plume expansion are shown to initiate vortex formation, followed by mixing dynamics that work to pull AlO into the vortices to react with gas-phase Al to form Al 2 O. Oxygen and several aluminum oxides are simultaneously pulled up through the stem of the fireball, encouraging further intermixing between reacting species and enhanced molecular formation. This work concludes that chemical dynamics in laser ablation plasmas is driven by diffusion processes, concentration gradients, and plume hydrodynamics while strong shockwaves generated during laser ablation do not impede chemical reactions.  more » « less
Award ID(s):
1905301
PAR ID:
10422731
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
Physical Chemistry Chemical Physics
Volume:
25
Issue:
23
ISSN:
1463-9076
Page Range / eLocation ID:
15666 to 15675
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ABSTRACT The chemistry of plasma–liquid interactions involves a complex interplay of physical and chemical processes at the plasma–liquid interface. These interactions give rise to the generation, transport, and transformation of various reactive species. Since the publication of the Lorenz Roadmap in 2016, significant progress has been made in understanding the interfacial transport and coupled reactions of plasma‐generated species with inorganic and organic compounds. However, critical aspects of plasma–liquid chemistry and mass transfer still require further investigation. This review summarizes recent work on processes at the plasma–liquid interface and the coupled reactions in the liquid phase. We highlight key findings related to the involvement of O atoms, H radicals, solvated electrons, photons, and nitrogen‐derived species at the interface and within the bulk liquid. 
    more » « less
  2. Aluminum monochloride (AlCl) has been proposed as a promising candidate for laser cooling to ultracold temperatures, and recent spectroscopy results support this prediction. It is challenging to produce large numbers of AlCl molecules because it is a highly reactive open-shell molecule and must be generated in situ . Here we show that pulsed-laser ablation of stable, non-toxic mixtures of Al with alkali or alkaline earth chlorides, denoted XCl n , can provide a robust and reliable source of cold AlCl molecules. Both the chemical identity of XCl n and the Al : XCl n molar ratio are varied, and the yield of AlCl is monitored using absorption spectroscopy in a cryogenic gas. For KCl, the production of Al and K atoms was also monitored. We model the AlCl production in the limits of nonequilibrium recombination dominated by first-encounter events. The non-equilibrium model is in agreement with the data and also reproduces the observed trend with different XCl n precursors. We find that AlCl production is limited by the solid-state densities of Al and Cl atoms and the recondensation of Al atoms in the ablation plume. We suggest future directions for optimizing the production of cold AlCl molecules using laser ablation. 
    more » « less
  3. Abstract In this work, a scalable and rapid process is developed for creating a low‐cost humidity sensor for wireless monitoring of moisture levels within packaged goods. The sensor comprises a moisture‐sensitive interdigitated capacitor connected to a planar spiral coil, forming an LC circuit whose resonant frequency is a function of environmental humidity. The sensor is fabricated on a commercially available metallized parchment paper through selective laser ablation of the laminated aluminum (Al) film on the parchment paper substrate. The laser ablation process provides a unique one‐step patterning of the conductive Al layer on the paper while simultaneously creating high surface area Al2O3nanoparticles within the laser‐ablated regions. The intrinsic humidity‐responsive characteristics of the laser‐induced Al2O3nanostructures provide the wireless sensor with a tenfold higher sensitivity to humidity than a similar LC resonant sensor prepared by conventional photolithography‐based processes on FR‐4 substrates. The frequency change of the sensor is observed to be a linear function within the range of 0−85% RH, providing an average sensitivity of −87 kHz RH−1with good repeatability and stable performance. Furthermore, the employment of scalable laser fabrication processes using commercially available inexpensive materials renders these technologies viable for roll‐to‐roll manufacturing of low‐cost wireless sensors for smart packaging applications. 
    more » « less
  4. Abstract Non-equilibrium inductively coupled plasmas (ICPs) operating in hydrogen are of significant interest for applications including large-area materials processing. Increasing control of spatial gas heating, which drives the formation of neutral species density gradients and the rate of gas-temperature-dependent reactions, is critical. In this study, we use 2D fluid-kinetic simulations with the Hybrid Plasma Equipment Model to investigate the spatially resolved production of atomic hydrogen in a low-pressure planar ICP operating in pure hydrogen (10–20 Pa or 0.075–0.15 Torr, 300 W). The reaction set incorporates self-consistent calculation of the spatially resolved gas temperature and 14 vibrationally excited states. We find that the formation of neutral-gas density gradients, which result from spatially non-uniform electrical power deposition at constant pressure, can drive significant variations in the vibrational distribution function and density of atomic hydrogen when gas heating is spatially resolved. This highlights the significance of spatial gas heating on the production of reactive species in relatively high-power-density plasma processing sources. 
    more » « less
  5. Abstract Plasmas interacting with liquid microdroplets are gaining momentum due to their ability to significantly enhance the reactivity transfer from the gas phase plasma to the liquid. This is, for example, critically important for efficiently decomposing organic pollutants in water. In this contribution, the role of ⋅ OH as well as non- ⋅ OH-driven chemistry initiated by the activation of small water microdroplets in a controlled environment by diffuse RF glow discharge in He with different gas admixtures (Ar, O 2 and humidified He) at atmospheric pressure is quantified. The effect of short-lived radicals such as O ⋅ and H ⋅ atoms, singlet delta oxygen (O 2 ( a 1 Δ g )), O 3 and metastable atoms of He and Ar, besides ⋅ OH radicals, on the decomposition of formate dissolved in droplets was analyzed using detailed plasma diagnostics, droplet characterization and ex situ chemical analysis of the treated droplets. The formate decomposition increased with increasing droplet residence time in the plasma, with ∼70% decomposition occurring within ∼15 ms of the plasma treatment time. The formate oxidation in the droplets is shown to be limited by the gas phase ⋅ OH flux at lower H 2 O concentrations with a significant enhancement in the formate decomposition at the lowest water concentration, attributed to e − /ion-induced reactions. However, the oxidation is diffusion limited in the liquid phase at higher gaseous ⋅ OH concentrations. The formate decomposition in He/O 2 plasma was similar, although with an order of magnitude higher O ⋅ radical density than the ⋅ OH density in the corresponding He/H 2 O plasma. Using a one-dimensional reaction–diffusion model, we showed that O 2 ( a 1 Δ g ) and O 3 did not play a significant role and the decomposition was due to O ⋅ , and possibly ⋅ OH generated in the vapor containing droplet-plasma boundary layer. 
    more » « less