Gas-phase oxidation and nanoparticle formation in multi-element laser ablation plumes

Kautz, Elizabeth J.; Zelenyuk, Alla; Gwalani, Bharat; Phillips, Mark C.; Harilal, S. S.

doi:10.1039/d2cp02437c

Cited by 5 publications

(4 citation statements)

References 40 publications

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“…Laser-ablation-based techniques are continuously making valuable contributions to the broader nuclear forensics research field in areas such as plasma surrogates for nuclear fireball chemistry discussed earlier in this review, as well as similarity of other phenomena between LA plasmas and nuclear fireballs, particularly radio-frequency generation, 392 particle formation, 75 and strong wave generation and interaction with the ambient environment that is partially discussed earlier in this review. 54,55 As always, additional research and development will advance the capabilities of these techniques, and it is possible that these advances improve the applicability of these techniques for nuclear forensics analysis and not just for elucidating fundamental phenomena that occur during and following a nuclear detonation.…”

Section: Two-dimensional Fluorescence Spectroscopymentioning

confidence: 99%

“…Plasma formation is a complex process that exhibits several key phenomena occurring over a large dynamic temporal range from 10 − 15 to 10 − 3 s, 73,75 such as laser–matter coupling, removal of material (ablation), plasma formation (breakdown), shockwave generation and propagation, and atomic recombination and cooling along with nanoparticle formation. 54,76–78 A study conducted by Wen et al 79 offers a time-lapse description of the physical phenomena involving laser coupling, plasma formation, and shockwave generation through a series of synchronized shadowgraphy and emission spectral images.…”

Section: Description Of a Laser Ablation Plasmamentioning

confidence: 99%

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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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Section: Two-dimensional Fluorescence Spectroscopymentioning

confidence: 99%

Section: Description Of a Laser Ablation Plasmamentioning

confidence: 99%

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

Kwapis,

Borrero,

Latty

et al. 2023

Appl Spectrosc

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“…Simple monoxides yield higher gas-phase polyatomic oxides that ultimately condense into nanoparticles that agglomerate into larger nanoclusters as the plasma cools. 9,10 Molecular information characterizing the sample material is key to understanding the composition of organics, oxidation, crystallinity, calcination, carbon content, precursor, etc. in that material.…”

Section: Introductionmentioning

confidence: 99%

“…Simple monoxides yield higher gas-phase polyatomic oxides that ultimately condense into nanoparticles that agglomerate into larger nanoclusters as the plasma cools. 9,10…”

Section: Introductionmentioning

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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