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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Outlook for active plasma spectroscopy with entangled two-photon absorption

Entangled two-photon absorption (ETPA) exhibits a quantum-enhanced two-photon absorption cross-section and a linear scaling with incident power that exceeds classical two-photon absorption (TPA) at low photon flux. Here, we assess the feasibility and applications of ETPA for active plasma spectroscopy. The ETPA-absorbed power for an Ar + species in a helicon plasma scenario is calculated to be as high as 0.6 nW cm −1 along the incident beam path for nondegenerate-entangled photon pairs that are near-resonant with an intermediate level. The ETPA absorption power exceeds classical TPA and Bremsstrahlung emission, a necessary condition for a feasible fluorescence measurement. Applications of ETPA plasma spectroscopy may include trace impurity detection, ground-state excitation, and continuous-wave pumping for high-bandwidth turbulence measurements. Possible benefits of plasma measurements are less harm to optical components with lower incident flux and reduced stray light that can contaminate optical diagnostics.

active plasma spectroscopy↗
DOE OSTI2020

Laser-Plasma Spectroscopy of Hydroxyl with Applications

This article discusses laser-induced laboratory-air plasma measurements and analysis of hydroxyl (OH) ultraviolet spectra. The computations of the OH spectra utilize line strength data that were developed previously and that are now communicated for the first time. The line strengths have been utilized extensively in interpretation of recorded molecular emission spectra and have been well-tested in laser-induced fluorescence applications for the purpose of temperature inferences from recorded data. Moreover, new experiments with Q-switched laser pulses illustrate occurrence of molecular recombination spectra for time delays of the order of several dozen of microseconds after plasma initiation. The OH signals occur due to the natural humidity in laboratory air. Centrifugal stretching of the Franck-Condon factors and r-centroids are included in the process of determining the line strengths that are communicated as a Supplementary File. Laser spectroscopy applications of detailed OH computations include laser-induced plasma and combustion analyses, to name but two applications. This work also includes literature references that address various diagnosis applications.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

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.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

VERITAS : A density-functional theory-based multiband kinetic model for understanding x-ray spectroscopy of dense plasmas

X-ray spectroscopy has long been a powerful diagnostic tool for hot, dilute plasmas, providing insights into plasma conditions by measuring line shifts and broadenings of atomic transitions. The technique critically depends on the accuracy of atomic physics models used to interpret spectroscopic measurements for inferring plasma properties such as free-electron density and temperature. Over the past decades, the atomic and plasma physics communities have developed robust atomic physics models to account for various processes in hot, dilute classical plasmas. While these models have been successful in that regime, their applicability becomes uncertain when interpreting x-ray spectroscopy experiments of above-solid-density plasmas. Given that finite-temperature density-functional theory (DFT) offers a more accurate description of dense plasma environments, we present the development of a DFT-based multi-band kinetic model, VERITAS, designed to improve the interpretation of x-ray spectroscopic measurements in high-density plasmas produced by laser-driven spherical implosions. This work details the VERITAS model and its application to both time-integrated and time-resolved x-ray spectra from implosion experiments on OMEGA. The advantages and limitations of the VERITAS model will also be discussed, along with potential directions for advancing x-ray spectroscopy of dense and superdense plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

Influence of thermal treatment on structure and catalytic performance of ceria-zirconia supported copper oxide (CuO x /Ce y Zr 1-y O 2 ) catalysts for CO oxidation

Copper oxide (CuO x ) supported on ceria-zirconia (Ce y Zr 1-y O 2 , y = 1.0, 0.5, 0.0) catalysts were investigated to elucidate the effects of thermal treatment on their physicochemical properties and catalytic performance in carbon monoxide (CO) oxidation. Here, the catalysts were synthesized via a one-pot chemical vapor deposition (OP-CVD) method at 700˚C and 900˚C with controlled Cu loading. Characterization techniques, including synchrotron X-ray diffraction (S-XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), inductively coupled plasma spectroscopy (ICP), and N 2 adsorption-desorption, were implemented to probe the crystalline structure, molecular and electronic structure, oxygen vacancies, specific surface area (SSA) and metal loading. CO oxidation was chosen as a model reaction to explore the structure-catalytic performance relationship. A ∼100% CO conversion was achieved at < 150˚C, particularly with the CuO x /CeO 2 catalyst calcined at 700˚C. In contrast, calcination at 900˚C caused a ∼90% decrease in SSA and a ∼24% increase in T 50 . Activity tests revealed that increasing ZrO 2 content lowered CO oxidation activity despite generating more defect sites. In-situ measurement of the 700 °C calcined samples revealed the presence of stable and unstable defects in CuO x /Ce 0.5 Zr 0.5 O 2 and CeO 2 respectively, which play a key role in the activity of the catalysts. The results highlight that catalytic performance is closely related to the SSA. Furthermore, an optimum calcination temperature favor significant oxygen vacancy formation with required CuO x -support interactions, enhancing redox properties and catalytic performance.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Laser-Plasma Spatiotemporal Cyanide Spectroscopy and Applications

This article reports new measurements of laser-induced plasma hypersonic expansion measurements of diatomic molecular cyanide (CN). Focused, high-peak-power 1064 nm Q-switched radiation of the order of 1 TW/cm 2 generated optical breakdown plasma in a cell containing a 1:1 molar gas mixture of N 2 and CO 2 at a fixed pressure of 1.1 × 10 5 Pascal and in a 100 mL/min flow of the mixture. Line-of-sight (LOS) analysis of recorded molecular spectra indicated the outgoing shockwave at expansion speeds well in excess of Mach 5. Spectra of atomic carbon confirmed increased electron density near the shockwave, and, equally, molecular CN spectra revealed higher excitation temperature near the shockwave. Results were consistent with corresponding high-speed shadowgraphs obtained by visualization with an effective shutter speed of 5 nanoseconds. In addition, LOS analysis and the application of integral inversion techniques allow inferences about the spatiotemporal plasma distribution.

36 MATERIALS SCIENCE↗
DOE OSTI2025

High-resolution spectroscopy of uranium laser-produced plasma using saturated absorption spectroscopy

High-resolution spectroscopy of laser ablation plumes or laser-produced plasmas (LPPs) is valuable for various applications, including measuring crowded spectral features, determining spectroscopic constants, characterizing plasmas, and performing isotopic analysis. However, various line broadening mechanisms in plasmas limit its use for several applications. Here, in this study, we present the use of saturated absorption spectroscopy (SAS) for Doppler-free linewidth analysis in a uranium LPP. We demonstrate that SAS is effective in obtaining Doppler-free Lamb dip profiles with linewidths on the order of ≤ 20 MHz. The effects of saturation on the Doppler-broadened absorption and Lamb dip profiles at different pressures and probe intensities are quantified, and their impact on measurements of plasma properties is discussed. Finally, we show that the linewidths of the Lamb dips can be used for quantitative estimates of pressure and natural broadening in the plasma.

Absorption spectroscopy↗
DOE OSTI2020

Cubic crystals in an x-ray polarization-splitting geometry

Hexagonal and cubic crystals contain paired sets of internal planes that reflect the linearly polarized components of certain x rays into two separate, perpendicular directions. For the cubic crystals, two distinct crystal orientations provide the same polarization-splitting geometry. One of the orientations may have advantages for plasma spectroscopy by suppressing unwanted reflections. This paper demonstrates the two orientations with a germanium crystal and K characteristic lines from copper and zirconium.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Mechanism of H 2 plasma-enabled reduction of hematite thin films

Hydrogen plasma is gaining significant interest as a promising pathway for direct iron ore reduction and for lowering process temperatures but the reduction mechanism remains poorly understood. In this work we analyzed the plasma and thermal reduction of thin-film hematite (Fe 2 O 3 ) at temperatures below 340 °C using X-ray diffraction and scanning electron microscopy with energy-dispersive X-ray spectroscopy. Plasma reduced the incubation period by an order of magnitude and increased the reduction rate by a factor of 2.6 compared to thermal reduction. Plasma-produced H-atoms facilitate the formation of numerous iron nucleation sites, bypassing the energetically unfavorable dissociative adsorption of H 2 on iron oxide. These iron nuclei can autocatalyze the reduction of the surrounding hematite via a hydrogen spillover mechanism. Our results demonstrate that plasma-derived H-atoms primarily impact the initial nucleation-limited stage. These new insights provide a mechanistic framework that can aid the implementation and optimization of hydrogen plasma-assisted iron oxide reduction at reduced temperatures.

08 HYDROGEN↗
DOE OSTI2023

Use of Electronic Laboratory Notebooks (ELN) in a Laboratory Information Management System (LIMS) [Slides]

The Actinide Analytical Chemistry (CAAC) group at Los Alamos National Laboratory (LANL) uses the LabWare LIMS (LabWare 7) system to manage our samples and material at risk. The LIMS system also provides other functionality which the Plasma Spectroscopy (PS) team has developed along with our LIMS team to provide streamlining and automation of all sample related actions required by PS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Application of helium line intensity ratio spectroscopy to xenon plasma in E × B Penning discharge

Here, we propose the application of helium line intensity ratio spectroscopy in a low-pressure (0.3 mTorr) xenon E × B discharge with an electron temperature of ~2 eV and a density of 10 10 –10 11 cm –3 . We successfully identified the helium atom line emissions at 388.9, 447.1, 501.6, 504.8, and 706.5 nm with helium pressures of up to ~20 mTorr. The measured electron temperature, density, and I–V characteristics of the discharge remained almost constant in all helium pressures in the present experiment, indicating the suitability of the helium gas as a diagnostic gas. The results of helium line intensity ratio spectroscopy using the line emissions at 388.9, 447.1, and 504.8 nm showed fair agreement with the Langmuir probe measurement. Considering the trade-off relationship between the disturbance introduced by the helium gas and the signal-to-noise ratio, we conclude that a helium pressure of approximately 4 mTorr (approximately 13 times the partial pressure of xenon) represents the optimal pressure range for the application of the helium line emission intensity ratio method to this xenon plasma. It is found that the use of the line emissions at 501.6 and 706.5 nm result in a significant disturbance in the helium line intensity ratio method due to the radiation trapping effect.

helium line intensity ratio spectroscopy↗
DOE OSTI2020

Trace Elemental Analysis of Bulk Thorium Using an Automated Separation–Inductively Coupled Plasma Optical Emission Spectroscopy Methodology

Presented here is a novel automated method for determining the trace element composition of bulk thorium by inductively coupled plasma–optical emission spectroscopy (ICP-OES). ICP-OES is a universal approach for measuring the trace elemental impurities present in actinide-rich materials; however, due to the emission rich spectrum of the actinide, a separation from the trace elements is warranted for spectrochemical analysis. Here, AG MP-1 ion exchange resin was utilized for retention of the Th matrix, while allowing the trace element impurities to be separated prior to subsequent analysis using ICP-OES. After demonstrating the separation on traditional gravity-driven columns, the methodology was transitioned to an automated platform for comparison. This automated platform utilizes syringe-driven sample and solvent flow and can collect the trace element and thorium fractions in separate locations. Finally, while reducing the sample size (500 µL, 1.5 mg of Th), maintaining the overall separation efficiency (recoveries >95%), and illustrating the sample throughput ability (n = 10+), this automated methodology could be readily adopted to nuclear facilities in which the determination of trace elemental impurities in Th samples is warranted.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Transuranium Sulfide via the Boron Chalcogen Mixture Method and Reversible Water Uptake in the NaCu T S 3 Family

The behavior of 5f electrons in soft ligand environments makes actinides, and especially transuranium chalcogenides, an intriguing class of materials for fundamental studies. Due to the affinity of actinides for oxygen, however, it is a challenge to synthesize actinide chalcogenides using non-metallic reagents. Using the Boron Chalcogen Mixture (BCM) method, we achieved the synthesis of the transuranium sulfide NaCuNpS 3 starting from the oxide reagent, NpO 2 . Via the same synthetic route, the isostructural composition of NaCuUS 3 was synthesized and the material contrasted with NaCuNpS 3 . Single crystals of the U-analog, NaCuUS 3 , were found to undergo an unexpected reversible hydration process to form NaCuUS 3 ·xH 2 O (x ≈ 1.5). Here, a large combination of techniques was used to fully characterize the structure, hydration process, and electronic structures, specifically a combination of single crystal, powder, high temperature powder X-ray diffraction, extended X-ray ab-sorption fine structure, infrared, and inductively coupled plasma spectroscopies, thermogravimetric analysis, and density functional theory calculations. The outcome of these analyses enabled us to determine the composition of NaCuUS 3 ·xH 2 O and obtain a structural model that demonstrated the retention of the local structure within the [CuUS 3 ] – layers throughout the hydration-dehydration process. Band structure, density of states, and Bader charge calculations for NaCuUS 3 , NaCu-US 3 ·xH 2 O, and NaCuNpS 3 along with X-ray absorption near edge structure, UV-vis-NIR and work function measurements on ACuUS 3 (A = Na, K, and Rb) and NaCuUS 3 ·xH 2 O samples were carried out to demonstrate that electronic properties arise from the [CuTS 3 ] – layers and show surprisingly little dependence on the interlayer distance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Atomic layer deposition for surface area determination of solid oxide electrodes

Surface area measurements are important for characterizing porous solids, but commonly used methods such as Brunauer–Emmett–Teller (BET) gas adsorption and computed nanotomography are lacking for certain applications such as the development of solid oxide fuel cell electrodes, which often have absolute surface areas <1 m 2 and contain nanoscale features. Presented is a novel method for the surface area determination of samples with total measurable areas of 1–1000 cm 2 with a standard deviation ± 1 cm 2 , utilizing the atomic layer deposition (ALD) of Al 2 O 3 over microstructurally complex internal porosity. The volume of alumina is then quantified using plasma spectroscopy and converted to an area using the known ALD layer thickness. Under the modest ALD reactor soak times used (8.5 s), the precursor penetration depth is found to be ~50 μm, exceeding the requirement for uniformly coating SOFC functional layers. A model system, (La 0.8 Sr 0.2 ) 0.98 MnO 3–δ /Ce 0.9 Gd 0.1 O 1.95 (LSM/GDC) scaffolds of ~2.7 m 2 g –1 , was measured using the technique and compared against the BET method, and comparable results were obtained but with 1000 times less material needed. The technique is demonstrated for measurements in two example areas of active SOFC research: exsolved (Ni, Fe) nanoparticles on an Sr(Ti, Fe, Ni)O 3–δ electrode and PrO x catalyst nanoparticles infiltrated onto LSM/GDC scaffolds. Finally, the technique may be broadly useful wherever the accurate surface area determination of small absolute quantities of porous ceramic structures on the order of 0.1–50 m 2 g –1 is sought.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Comparison of excitation and kinetic temperatures in a laser-produced plasma using absorption spectroscopy

High-resolution tunable laser absorption spectroscopy is used to measure time-resolved absorption spectra for six neutral uranium transitions in a laser-produced plasma. Here analysis of the spectra shows that kinetic temperatures are similar for all six transitions, but excitation temperatures are higher than kinetic temperatures from 10–100 μs, indicating departures from local thermodynamic equilibrium.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Elemental Analysis of Bio-Oils by Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES). Laboratory Analytical Procedure (LAP), Issue Date: May 13, 2022

Concentrations of inorganic elements is a key quality metric for bio-oils as certain elements impact upgrading processes and product quality. Unless reduced or removed during production and processing, alkali and alkaline metals native to lignocellulosic biomass can carry over into bio-oils contributing to ash content and degraded catalyst performance during upgrading to hydrocarbon fuels or chemical products. Non-metallic elements such as sulfur and phosphorus can also negatively impact upgrading catalysts and product quality. Inductively coupled plasma optical emission spectroscopy (ICP-OES) can be used to measure inorganic elements of interest in bio-oils. This procedure covers the preparation and analysis of fast pyrolysis (FP) and catalytic fast pyrolysis (CFP) bio-oils. The concentrations of these elements can indicate potential bio-oil quality from the perspective of deoxygenation processes. The implications of elemental composition will depend on process parameters such as upgrading catalyst sensitivities. This Laboratory Analytical Procedure (LAP) covers two methods for quantification of inorganic elements by ICP-OES: Procedure A uses microwave assisted digestion with concentrated nitric acid, and Procedure B is an organic ICP-OES method utilizing a diglyme solvent.

09 BIOMASS FUELS↗