Effects of Plume Hydrodynamics and Oxidation on the Composition of a Condensing Laser-Induced Plasma

Weisz, David G.; Crowhurst, Jonathan C.; Finko, Mikhail; Rose, Timothy P.; Köroğlu, Batikan; Trappitsch, R.; Radousky, Harry B.; Siekhaus, Wigbert J.; Armstrong, Michael R.; Isselhardt, Brett H.; Azer, Magdi; Curreli, Davide

doi:10.1021/acs.jpca.7b11994

Cited by 25 publications

(11 citation statements)

References 36 publications

(85 reference statements)

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“…Molecules characterized by higher dissociation energies form at earlier times in the plasma plume when temperature conditions are hotter. 29,30…”

Section: Resultsmentioning

confidence: 99%

Laser-Induced Plasmas of Plutonium Dioxide in a Double-Walled Cell

Villa-Aleman,

Kwapis,

Foley

et al. 2024

Appl Spectrosc

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Plutonium research has been stifled by the significant number of administrative controls and safety procedures, space and instrumentation limitations in radiological gloveboxes, and the potential for personnel and equipment contamination. To address the limited number of spectroscopic studies in Pu-bearing compounds in the current scientific literature, this work presents the use of double-walled cells (DWCs) in “clean” buildings/laboratories as an alternative to research in radiological gloveboxes. This study reports the first laser-induced breakdown spectroscopy (LIBS) experiments of a PuO2 pellet contained within a DWC, where the formation of elemental (atomic and ionic) species as well as the evolution from elemental to molecular products (Pu xO y) was measured. Raman spectroscopy was also used to characterize the surface of the ablated pellet and the particulates deposited on the window of the inner cell. The full width half-maximum of the T2g band enabled us to obtain an estimate of the temperature at the pellet surface after the ablation pulse and the particulates based on the crystal lattice disorder. Particulates deposited on the window of the DWC during laser ablation were characterized using scanning electron microscopy, where molten irregular particulates and spheroids were observed. This exciting research conducted in a DWC describes our initial attempts to incorporate LIBS in the arsenal of spectroscopic tools for nuclear forensics applications.

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“…Molecules characterized by higher dissociation energies form at earlier times in the plasma plume when temperature conditions are hotter. 29,30…”

Section: Resultsmentioning

confidence: 99%

Laser-Induced Plasmas of Plutonium Dioxide in a Double-Walled Cell

Villa-Aleman,

Kwapis,

Foley

et al. 2024

Appl Spectrosc

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“…71 Using time-resolved, fast-gated imaging with bandpass filters, this behavior has been demonstrated experimentally with the ablation of a SrZrO 3 target; ZrO ( D 0 = 7.8 eV) was observed to form volumetrically and at earlier times in the plasma than SrO ( D 0 = 4.9 eV), while SrO was predominantly distributed in the cooler plasma periphery. 139 Furthermore, monoxides in aluminum LPPs ( D 0 , .1em AlO = 5.3 eV) have been measured to form at the interface between the plasma and ambient gas, 128 while those in uranium LPPs ( D 0 , .1em UO = 7.9 eV) have been observed to coexist in the plasma core with U I. 140…”

Section: Laser Ablation Plasma Chemistrymentioning

confidence: 99%

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

Kwapis,

Borrero,

Latty

et al. 2023

Appl Spectrosc

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The development of measurement methodologies to detect and monitor nuclear-relevant materials remains a consistent and significant interest across the nuclear energy, nonproliferation, safeguards, and forensics communities. Optical spectroscopy of laser-produced plasmas is becoming an increasingly popular diagnostic technique to measure radiological and nuclear materials in the field without sample preparation, where current capabilities encompass the standoff, isotopically resolved and phase-identifiable (e.g., UO and UO[Formula: see text]) detection of elements across the periodic table. These methods rely on the process of laser ablation (LA), where a high-powered pulsed laser is used to excite a sample (solid, liquid, or gas) into a luminous microplasma that rapidly undergoes de-excitation through the emission of electromagnetic radiation, which serves as a spectroscopic fingerprint for that sample. This review focuses on LA plasmas and spectroscopy for nuclear applications, covering topics from the wide-area environmental sampling and atmospheric sensing of radionuclides to recent implementations of multivariate machine learning methods that work to enable the real-time analysis of spectrochemical measurements with an emphasis on fundamental research and development activities over the past two decades. Background on the physical breakdown mechanisms and interactions of matter with nanosecond and ultrafast laser pulses that lead to the generation of laser-produced microplasmas is provided, followed by a description of the transient spatiotemporal plasma conditions that control the behavior of spectroscopic signatures recorded by analytical methods in atomic and molecular spectroscopy. High-temperature chemical and thermodynamic processes governing reactive LA plasmas are also examined alongside investigations into the condensation pathways of the plasma, which are believed to serve as chemical surrogates for fallout particles formed in nuclear fireballs. Laser-supported absorption waves and laser-induced shockwaves that accompany LA plasmas are also discussed, which could provide insights into atmospheric ionization phenomena from strong shocks following nuclear detonations. Furthermore, the standoff detection of trace radioactive aerosols and fission gases is reviewed in the context of monitoring atmospheric radiation plumes and off-gas streams of molten salt reactors. Finally, concluding remarks will present future outlooks on the role of LA plasma spectroscopy in the nuclear community.

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“…This capability is useful in LIBS and LAMIS experiments. It is known that emission from atoms, ions, and molecules is observed at different times and in different regions of the laser-induced plasma [6,[22][23][24]. In general, the intensity of atomic emission increases with distance from the sample surface, where it eventually reaches a maximum emission value (e.g., between 0.5 mm and 1.5 mm for a copper sample depending on laser irradiance) and decreases at longer distance (e.g., starting from maximum emission to between 1.5 mm to 3.0 mm depending on laser irradiance) from the surface [4].…”

Section: Spatial Filteringmentioning

confidence: 99%

“…The locations highest above the sample surface show the greatest emission from YO which would correspond to the area with the most interaction with ambient environment. The spatial emission profile of Y emission reveals the quick dissipation of the Y atomic and ionic emission and the persistence of the YO emission bands which are due to the formation of the YO species due to interactions with atmospheric gases, rather than YO being ablated from the surface of the Y sample [22][23][24]26].…”

mentioning

confidence: 99%