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DOE OSTI2024

Argon metastable density and temperature of a 94 GHz microplasma

Laser diode absorption spectroscopy is used to experimentally measure Ar(1s 5 ) metastable density and translational gas temperature within a 94 GHz microplasma. A square two-dimensional photonic crystal (PhC) at this resonance frequency serves to ignite and sustain the plasma from 20 to 200 Torr (2.7 × 10 3 –2.7 × 10 4 Pa) by using millimeter wave power from 300 to 1000 mW. Metastable density within the plasma is estimated from the absorption line shape of the laser traversing the PhC. The metastable density reaches an order of 10 19 m –3 at lower pressure and decreases as pressure increases. From the Lorentzian line shape of the absorption profile at 811.53 nm, the gas temperature is extracted and found to increase from 500 K at 20 Torr to 1300 K at 200 Torr. Furthermore, these data are analyzed and compared with a zero-dimensional plasma model and with previous experimental plasma results at 43 GHz.

42 ENGINEERING↗

DOE OSTI2025

X-ray Absorption Spectroscopy of Dilute Metalloenzymes at X-ray Free-Electron Lasers in a Shot-by-Shot Mode

X-ray absorption spectroscopy (XAS) of 3d transition metals provides important electronic structure information for many fields. However, X-ray-induced radiation damage under physiological temperature has prevented using this method to study dilute aqueous systems, such as metalloenzymes, as the catalytic reaction proceeds. Here we present a new approach to enable operando XAS of dilute biological samples and demonstrate its feasibility with K-edge XAS spectra from the Mn cluster in photosystem II and the Fe–S centers in photosystem I. This approach combines highly efficient sample delivery strategies and a robust signal normalization method with high-transmission Bragg diffraction-based spectrometers at X-ray free-electron lasers (XFELs) in a damage-free, shot-by-shot mode. These photon-out spectrometers have been optimized for discriminating the metal Mn/Fe Kα fluorescence signals from the overwhelming scattering background present on currently available detectors for XFELs that lack suitable energy discrimination. We quantify the enhanced performance metrics of the spectrometer and discuss its potential applications for acquiring time-resolved XAS spectra of biological samples during their reactions at XFELs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Relativistic coupled-cluster calculations of RaOH pertinent to spectroscopic detection and laser cooling

Here a relativistic coupled-cluster study of the low-lying electronic states in the radium monohydroxide molecule (RaOH), a radioactive polyatomic molecule of interest to laser cooling and to the search of new physics beyond the Standard Model, is reported. The level positions of the A 2 Π 1/2 and C 2 Σ states have been computed with an accuracy of around 200 cm –1 to facilitate spectroscopic observation of RaOH using laser induced fluorescence spectroscopy, thereby exploiting the systematic convergence of electron-correlation and basis-set effects in relativistic coupled-cluster calculations. The energy level for the B 2 Δ 3/2 state has also been calculated accurately to conclude that the B 2 Δ 3/2 state lies above the A 2 Π 1/2 state. This confirms X 2 Σ ↔ A 2 Π 1/2 as a promising optical cycling transition for laser cooling RaOH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Online LIBS–ML Framework for Dynamic Characterization of Heterogeneous Waste-Derived Gasification Feedstocks

LIBS−ML framework for real time feedstock characterization during continuous conveyor transport Heterogeneous waste derived feedstocks (e.g., waste coal, biomass and blends) introduce rapid variability in heating value and ash chemistry that affect gasifier operation, yet conventional laboratory characterization techniques are too slow to support proactive control. To address this gap, this study reports on an online, in situ, dynamic characterization framework that couple’s laser-induced breakdown spectroscopy (LIBS) with leakage safe machine learning (ML) regression to deliver real time, decision quality predictions of gasifier relevant properties. A controlled sample matrix spanning two different waste coals, two different biomasses, and engineered blends under two particle size conditions were constructed and benchmarked using standardized laboratory analyses for proximate/ultimate properties and ash composition. LIBS spectra were acquired dynamically as material flowed on a conveyor belt, using high energy 1064 nm laser ablation and shot averaging to improve repeatability and precision. Supervised regression models (multi layer perceptron (MLP) /artificial neural network (ANN), random forest (RF), and support vector regression (SVR)) and an optimized weighted ensemble were trained on emission line feature sets using nested cross validation with Bayesian hyperparameter tuning and validated against an independent hold out set. The proposed LIBS−ML workflow achieves near laboratory predictive fidelity across parametric targets (including higher heating value (HHV), ash content, fixed carbon, sulfur, major ash forming oxides, and initial deformation temperature (IDT)), with the weighted ensemble providing a robust default predictor under dynamic measurement conditions. These results demonstrate a practical pathway for real time feedstock characterization that can enable feedforward adjustments and more resilient gasifier operation for variable quality waste derived fuels.

Biomass↗

DOE OSTI2024

A Molten Salt Aerosol Spectroscopy Approach to Online Process Monitoring in Molten Salt Reactors

Recent research and development in molten salt reactors (MSRs) has led to many advanced reactor designs, many of which have demonstrations planned in the next decade. However, a significant challenge that must be overcome before liquid fueled MSRs become viable globally is nuclear material accountancy (NMA) and safeguards. Liquid-fueled MSRs are problematic to safeguards because the nuclear material is in the bulk phase, inventories are constantly changing, and there are potentially many outlet pathways that must be monitored, especially in designs with online chemical processing. At the Idaho National Laboratory, we have developed a process monitoring tool to circulate molten salt through a nebulizer and optical cell, where laser-induced breakdown spectroscopy (LIBS) and ultraviolet-visible (UV-VIS) are applied to track the elemental and oxidation states of the constituents in the salt aerosol. This approach has the potential to provide information on the actinides, fission products, and corrosion in the reactor or process. Preliminary testing in aqueous praseodymium chloride (PrCl3) and neodymium chloride (NdCl3) showed good sensitivity detection limits n developed calibration curves. Additional tests and analysis or ongoing in aqueous solutions while equipment is being scaled up for high temperature molten salt testing. Results for continued testing as well as a status of the molten salt design and anticipated commissioning will be presented.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2026

Burst delay line for generating ultrashort pulse bursts with interval tunability from femtoseconds to nanoseconds.

Ultrashort burst laser pulses are important for applications in laser processing and spectroscopy. However, existing burst generators face limitations in pulse time interval tunability and coaxiality. Here, we present a burst pulse generator that delivers coaxial ultrashort pulses with tunable pulse time intervals using a single translation stage. The constructed system produced eight femtosecond pulses with uniform intervals tunable from 100 fs to 1.93 ns, equivalent to burst-internal repetition rates spanning 10 THz to 0.52 GHz. We further demonstrated interval-dependent plasma emission in air filamentation, providing a compact platform to study burst-laser-induced phenomena.

Shimada, Keitaro↗

DOE OSTI2024

Spatiotemporal characterization of cerium monoxide in laser ablation plasmas using spectrally-resolved fast-gated imaging

The impact of oxidation chemistry on the emission characteristics and spatial structure of laser-produced Ce metal plasmas was investigated using laser-induced breakdown spectroscopy (LIBS) and time-resolved fast-gated imaging employing narrowband optical filters. Images of the plasma emission show that CeO coexists with atomic species in the periphery and vortex ring of the plasma plume. Image processing was also applied to combine independent monochromatic images of the plasma emission into a single merged image, culminating in a timelapse on the spatiotemporal evolution of atomic and molecular species within the plasma plume. The formation of CeO species was observed to proceed faster for plasmas generated in atmospheres containing larger concentrations of oxygen based on ratios of CeO-to-atomic emission intensities. Furthermore, these same ratios were shown to plateau and decrease at later times (≥25 μs), potentially indicating the depletion of CeO number densities in the plasma as the monoxide undergoes reactions to form higher polyatomic oxides. Altogether, these results provide fundamental insights into the chemical dynamics and intermixing between plasma-gas species in laser ablation cerium plasmas, advancing our understanding on optical signatures of nuclear-relevant materials to enable in-field measurement capabilities.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Emission phases of implosion sources for x-ray absorption fine structure spectroscopy

At the Laboratory for Laser Energetics' Omega Laser Facility, thin plastic shells were directly driven with ∼20 kJ resulting in a time-integrated x-ray yield of ∼1012 ph/eV/sr at 7 keV. Using temporally, spatially, and spectrally discriminating diagnostics, three x-ray emission phases were identified: corona emission produced by the laser ablation of the shell, core stagnation, and afterglow emission due to the expanding hot material after stagnation. The newly measured corona and afterglow emission phases account for ∼25% of the total x-ray signal and produce x-ray emission at a different time or larger radius than previously considered. The resulting implications of this additional emission for x-ray absorption fine structure spectroscopy are discussed. Finally, improvements to the laser drive intensity and uniformity produced a factor-of-2 increase in total x-ray emission while decreasing the size of the stagnated core.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

One-colour (~220 nm) resonance-enhanced (S 1 –S 0 ) multi-photon dissociation of acetylene: probe of the C 2 A 1 Π u – X 1 Σ + g band by frequency-modulation spectroscopy

In a recent paper, we demonstrated that one-colour (~220 nm), resonance-enhanced (S 1 –S 0 ), photodissociation of acetylene generates strong $C_2$ Swan band ($d^3Π_g–a^3Π_u$) and $C_2$ Deslandres-d'Azambuja band ($C^1Π_g–A^1Π_u$) fluorescence, and long-lived (>3 µs) fluorescence from an electronically-excited $C_2$H * species. It was not known whether the $C_2A^1Π_u$ and $X^1Σ^+_g$ states are also directly populated in this process. In this paper, multiple vibration-rotation transitions between the $C_2A$-state v = 2 and the X-state v = 0 level are examined by time-resolved frequency-modulation (FM) spectroscopy. The photolysis laser wavelength is tuned into resonance at the one-photon level with S 1 –S 0 transitions that populate individual rotational levels of the S 1 $_{trans}$-conformer $3^2,3^3,$ and $3^4$ vibrational states. By comparing the phase of the FM signals from the $C_2A–X$ transitions with that from the Rb D 1 -line absorption transition, we determine that, for all of the probed A–X transitions, the X-state level is more populated than the A-state level. We propose that the acetylene S 1 level is excited by the second photon to an acetylene dissociation precursor state, which undergoes sequential C-H bond-breaking to produce the $C_2X$ state. The dissociation precursor is assigned as the $1^1B_g(trans-bent)/1^1B_1(cis-bent)$ valence state, which correlates to a doubly-excited configuration, $(1π_u)^2(1π_g)^2$, at linear geometry. Based on the rotational distributions of the $C_2X$-state fragments, we believe that at least one of the transition states involved in the photolysis via S 1 $3^4$ has a larger CC-H bend-angle for the departing H-atom than that involved in the S 1 $3^2$ and $3^3$ photolysis.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

SuperCam Calibration Targets: Design and Development

Abstract SuperCam is a highly integrated remote-sensing instrumental suite for NASA’s Mars 2020 mission. It consists of a co-aligned combination of Laser-Induced Breakdown Spectroscopy (LIBS), Time-Resolved Raman and Luminescence (TRR/L), Visible and Infrared Spectroscopy (VISIR), together with sound recording (MIC) and high-magnification imaging techniques (RMI). They provide information on the mineralogy, geochemistry and mineral context around the Perseverance Rover. The calibration of this complex suite is a major challenge. Not only does each technique require its own standards or references, their combination also introduces new requirements to obtain optimal scientific output. Elemental composition, molecular vibrational features, fluorescence, morphology and texture provide a full picture of the sample with spectral information that needs to be co-aligned, correlated, and individually calibrated. The resulting hardware includes different kinds of targets, each one covering different needs of the instrument. Standards for imaging calibration, geological samples for mineral identification and chemometric calculations or spectral references to calibrate and evaluate the health of the instrument, are all included in the SuperCam Calibration Target (SCCT). The system also includes a specifically designed assembly in which the samples are mounted. This hardware allows the targets to survive the harsh environmental conditions of the launch, cruise, landing and operation on Mars during the whole mission. Here we summarize the design, development, integration, verification and functional testing of the SCCT. This work includes some key results obtained to verify the scientific outcome of the SuperCam system.

Manrique, J. A. (ORCID:0000000220532819)↗

DOE OSTI2021

The SuperCam Instrument Suite on the Mars 2020 Rover: Science Objectives and Mast-Unit Description

On the NASA 2020 rover mission to Jezero crater, the remote determination of the texture, mineralogy and chemistry of rocks is essential to quickly and thoroughly characterize an area and to optimize the selection of samples for return to Earth. As part of the Perseverance payload, SuperCam is a suite of five techniques that provide critical and complementary observations via Laser-Induced Breakdown Spectroscopy (LIBS), Time-Resolved Raman and Luminescence (TRR/L), visible and near-infrared spectroscopy (VISIR), high-resolution color imaging (RMI), and acoustic recording (MIC). SuperCam operates at remote distances, primarily 2–7 m, while providing data at sub-mm to mm scales. We report on SuperCam’s science objectives in the context of the Mars 2020 mission goals and ways the different techniques can address these questions. The instrument is made up of three separate subsystems: the Mast Unit is designed and built in France; the Body Unit is provided by the United States; the calibration target holder is contributed by Spain, and the targets themselves by the entire science team. This publication focuses on the design, development, and tests of the Mast Unit; companion papers describe the other units. The goal of this work is to provide an understanding of the technical choices made, the constraints that were imposed, and ultimately the validated performance of the flight model as it leaves Earth, and it will serve as the foundation for Mars operations and future processing of the data.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Boron adsorption in clay minerals: Implications for martian groundwater chemistry and boron on Mars

Boron has been detected on Mars in calcium-sulfate veins found within clay mineral rich rocks on Mars by the Mars Science Laboratory (MSL) Curiosity rover using Laser Induced Breakdown Spectroscopy (LIBS) analysis. Borates play a vital role in stabilizing ribose on Earth and has been suggested as a key requirement for life. Borate ions readily adsorb to phyllosilicate clay minerals. The discovery of boron on Mars in proximity to phyllosilicate-bearing bedrock may have strong implications for potential past prebiotic conditions on Mars. In this study we generated a suite of clay minerals with adsorbed borate, including both typical terrestrial clay minerals (montmorillonite) and Mars-analog clay minerals (nontronite, saponite, griffithite), to understand controls on borate adsorption and to analyze with LIBS to compare with MSL data. Clay minerals were subjected to mineralogical and chemical analysis before and after adsorption. Adsorption analysis revealed that the Mars analog clay minerals adsorbed less boron than terrestrial counterparts, but within comparable amounts to those detected on Mars and in meteorites. Post-adsorption analysis by X-ray diffraction (XRD) revealed slight changes in the interlayer spacing of many of the clay minerals. Based on the adsorption analysis of the Mars-analog clay minerals, phyllosilicate-bearing bedrock in Gale crater may contain up to 90-110 ppm B. A series of borate-enriched samples were created for analysis of LIBS spectra from ChemCam on the Curiosity rover and SuperCam on the Perseverance Rover. Finally, the results of this study may provide insight into martian groundwater geochemistry processes and the mobility of a key molecule connected with life.

58 GEOSCIENCES↗

DOE OSTI2025

Enhancing low-temperature sintering in the MgO-LiF system: Mechanistic insights

In the present article, we provide compelling evidence that minor (1 wt%) additions of micron and nanometre-sized LiF particles in MgO decompose leading to free Li diffusing into MgO surfaces enhancing vacancy production during direct current sintering. The addition of nanometre-sized LiF particles leads to a > 500 °C reduction in the sintering temperature and over 99 % theoretical density of final consolidated compacts. Correlating differential scanning calorimetry with in-situ x-ray diffraction, together with Schottky calculations, post sintering electron microscopy and laser induced breakdown spectroscopy, we uncover critical insights into this impressive reduction in sintering temperature. Our quantitative analysis reveals that MgO and LiF interact at low temperatures with the diffusion of Li into the surface of MgO particles due to the intrinsic structural disorder of the LiF and MgO crystallites. Nanometre-sized LiF particles were found to react the most at low temperatures due to their increased structural disorder. Our multimodal characterization points to a Li-promoted densification and sintering mechanism. This impressive reduction in sintering temperature can be harnessed to promote low-temperature fabrication of MgO-based composites for technological applications.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Shock tube/laser absorption measurement of the rate constant of the reaction: H 2 O 2 + CO 2 2OH + CO 2

We address the role of the linear mixing rule in the kinetics of the H 2 O 2 decomposition system by reporting the rate constant for H 2 O 2 + M = 2OH + M (M = Ar and CO 2 ) in the temperature range of 1087-1234 K at low pressures in a mixture of 20% CO 2 in Argon. The reaction rate constant was inferred from H 2 O concentrations monitored by using a laser-absorption spectroscopy-based water diagnostic. To the best of our knowledge, this is the first measurement of the rate constant of this reaction in a mixture to be reported in literature. A significant discrepancy was found between the rate constants derived using the traditional linear mixing rule and the reduced pressure linear mixing rule. Furthermore, this discrepancy can have serious implications on the predictive accuracy of these kinetic models, especially under conditions relevant to the operation of supercritical CO 2 (sCO 2 ) power cycles that rely on oxy-fuel combustion in a working fluid comprised almost entirely of CO 2 .

20 FOSSIL-FUELED POWER PLANTS↗

DOE OSTI2021

Improving ChemCam LIBS long-distance elemental compositions using empirical abundance trends

The ChemCam instrument on the Curiosity rover provides chemical compositions of Martian rocks and soils using remote laser-induced breakdown spectroscopy (LIBS). The elemental calibration is stable as a function of distance for Ti, Fe, Mg, and Ca. The calibration shows small, systematically increasing abundance trends as a function of distance for Al, Na, K, and to some extent, Si. The distance effect is known to be due to a dependence with distance on the relative strengths of atomic transition lines. Emission lines representing transitions from relatively low energy levels remain intense at longer distances while emission lines representing transitions from higher energy levels decrease in intensity more rapidly as a function of distance. The multivariate algorithms used to determine elemental compositions rely on a large number of emission lines in many cases, so rather than trying to correct all emission lines, a study was made of the predicted compositions as a function of distance, in order to determine an empirical correction. Abundance trends can be well approximated by a linear trend with distance within the ranges of abundances and distances observed up to ~6 m. Data from 11 distinct geological members and data groups of the Murray formation in Gale crater, Mars, were used to form the model, selecting the members and data groups yielding the best statistics. The model was tested using data from several targets observed from two different distances, and using data from the Kimberley formation, the composition of which is significantly different from the Murray formation, showing that the model works on other compositions beyond those used to build the model. For long-distance observations up to ~6 m, corrections can be made back to an equivalent composition at the median distance of ChemCam observations (2.6 m). Finally, the model has been validated up to 6.2 m, although ChemCam is able to observe bedrock targets to >7 m, and iron meteorites to distances of >9 m.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

A data analysis method to rapidly characterize gallium concentration in plutonium matrices using LIBS

The processing of actinide samples is a complex and costly endeavor that requires compositional analysis at various stages. Laser-induced breakdown spectroscopy (LIBS) has been used to analyze actinide-containing samples in many nuclear applications including waste management, fuel processing and forensics. The LIBS spectrum obtained from actinide materials are generally extremely complex, exhibiting many thousands of strong emission lines. This makes it difficult to identify other elements within the sample of interest, given the rich and dominant actinide spectrum. Here, in this article, we describe a recent effort to identify and quantify impurities and alloying constituents in plutonium matrices using a hand-held LIBS instrument that is used to rapidly and efficiently measure an emission spectrum from a material sample. We tabulate the emission line positions and intensities of plutonium. We report the development of machine-learning software that can identify gallium and quantify its concentration in plutonium matrices. This work has the potential to provide a rapid and nearly non-destructive technique that allows more confidence in characterizing the composition of materials that are present within complex actinide associated targets. We describe how our LIBS measurements and data analysis methods have successfully quantified the gallium concentration in a variety of samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Ensemble methods for quantification of potassium oxide in ChemCam Mars and laboratory spectra

In this paper we test new approaches for predicting the amount of element oxides in rock samples from the ChemCam instrument suite onboard the NASA Curiosity rover by focusing on K 2 O. Using the expanded dataset compiled by Gasda et al. (2021) with and without the Earth to Mars (E2M and NoE2M) transformation discussed in Clegg et al. (2017) we trained blended submodels using the “double blending” technique and compared these to ensemble methods (Random Forest, ExtraTrees, and Gradient Boosting Regression). We found that ensemble methods performed similar to blended submodels when looking at RMSE-P on the laboratory spectra and provided significant advantages when looking at spectra coming from Mars. For the full model, blended submodels achieved an RMSE-P of 0.62 and 0.60 (E2M and NoE2M respectively) while Gradient Boosting Regression resulted in a slightly improved RMSE-P of 0.59 and 0.60. More importantly, by employing a local RMSE-P estimation technique where model performance is evaluated based on nearby test samples we found that using ensemble methods can lower the quantification limit for K 2 O from the current value of ≈0.6 wt% to ≈0.08 wt% using Extra Trees and Random Forest. This would allow for a much larger range of K 2 O values to be quantified on Mars with greater certainty given that most targets seen on Mars tend to have <1 wt% K2O. Finally, we used both Mean Decrease in Impurity (MDI) and permutation importance techniques to investigate the wavelengths used by the ensemble methods and found that they correspond to known potassium emission lines. This suggests that ensemble methods can provide an easier to train and improved alternative to blended submodels for predicting potassium compositions from Laser Induced Breakdown Spectroscopy (LIBS) data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Development and demonstration of a rolling ball viscometer for molten salts with near-minimum liquidus NaCl–KCl

The thermophysical characterization of molten chloride and fluoride salts is a key interest for the development of advanced molten salt nuclear reactors. Viscosity is one thermophysical property of interest; a high-accuracy understanding of this property is necessary for modeling the thermal energy transfer and mass flow rate for a given molten salt system. Only a few methods have consistently been used to measure the viscosity of molten chloride and fluoride salt systems, and large discrepancies have been observed in the literature between independent studies of nearly identical salt systems. As such, exploration of novel measurement methods or implementations may allow for further validation, improved measurement accuracy, and overall improved understanding about optimal approaches for measuring molten salt viscosity. Here, in this study, a novel implementation of the rolling ball viscometry method was used to measure the viscosity of a 44/56 mol % mixture of NaCl–KCl within a temperature range of 714–838 °C, with the intent to demonstrate the feasibility of this technique for molten salt viscosity measurement cross-validation. The purity of this salt was confirmed through laser-induced breakdown spectroscopy. Measured viscosities were approximately 1.3–1.0 cP within this temperature range, and the overall uncertainty was 10.8%, which was determined through Gaussian error propagation. The results agree reasonably well with measured viscosities of similar NaCl–KCl mixtures in the literature (within 2%–20% depending on the temperature and study), although the experimental error in some of these comparative studies may be significant.

47 OTHER INSTRUMENTATION↗