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At least 37 records · Page 2

Development of a Versatile Analysis Method for the Isotopic Characterization of Alpha Spectra

Over the past several years significant work has been performed at Idaho National Laboratory to build an alpha-particle spectrometry capability and expertise for a wide range of applications that include technical nuclear forensics, nuclear safeguards, and environmental monitoring. This development has led to a diverse collection of sample types and preparations measured with varied solid-state detector materials and configurations. Several characteristics of a measured alpha pulse height spectrum make performing localized fits of individual peak shapes unfeasible. Alternatively, the entirety of the spectrum must be fit concurrently to extract isotopic information. An analysis tool has been developed to perform isotopic characterization of alpha spectra. This process included a study of both the mathematical model used to represent the detector response of an alpha-particle as well as the algorithm used to fit the spectrum.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Actinide in Air (Rn-Progeny Rejected) Alpha Spectroscopy With Tensioned Metastable Fluid Detectors

Here, this article discusses outcome of research for deriving a methodology and apparatus for ascertaining for the presence of ultratrace-level actinides in air from their alpha emission signatures, while remaining blind to the relatively large (1000× higher activity) alpha emissions from Rn-progeny. Apparatus and techniques were developed to collect and characterize alpha-emitting nuclides of Rn-progeny and actinides in air on a polycarbonate 3 μm pore size continuous air monitor (CAM) filter. A wet-chemistry approach was developed and validated for successfully separating the Rn-progeny alpha emitting isotopes of Po-214 and Po-218, while extracting the actinides (U, Pu, Am) in a fluid mixture that is suitable for conduct of alpha spectroscopy with a centrifugally tensioned metastable fluid detector (CTMFD). The resulting α-TMFD technology was compared against the state-of-art “Alpha-Sentry™” Continuous Air Monitor (CAM) system commonly utilized world-wide. Results indicate that the α-TMFD technology can potentially offer complementary and superior performance in multiple performance categories, and ∼18× improvement in the time to detect (e.g., at 0.02 derived air concentration (DAC) within ∼3 h, versus ∼70 h for Alpha-Sentry) for actinides of interest while also remaining ∼100% blind to ∼10 3 × higher Rn-progeny background—with the added potential for offering few keV scale energy resolution without resorting to peak shape fitting, versus ∼300–400 keV for existing CAM systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

R3 FLASHTALK - FASTPAC -- July 2022

This is a brief slide deck to provide our project team an update on our FASTPAC project for NA-22.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Tensioned metastable fluid detector sensing technology for multifarious-multiscale applications in the nuclear fuel cycle

The nuclear fuel cycle presents formidable 10 30+ multiscale challenges for high-efficiency spectroscopic sensing of alpha-neutron-fission radiation signatures amidst extreme gamma-beta radiation backgrounds at various stages of the cycle; it involves diverse arenas ranging from continuous/pulsed power production, security/safeguards, spent fuel, environmental remediation, and personnel health-dosimetry. This paper discusses the novel tensioned metastable fluid detector (TMFD) sensor technology. It discusses the results of studies demonstrating extreme (10 4 Sv/h) gamma-beta field blind high intrinsic efficiencies (80–100%) for neutron-alpha-fission radiation spectrometric detection. Example studies discussed in this paper include Neutron detection with spectroscopy; H*10 neutron radiation dosimetry upwards from ultra-low10 −2 µSv/h levels; Air and/or liquid-borne trace (10 –3 Bq/mL) quantity, 1 keV energy resolved alpha/fission spectroscopy for Rn/Po/U/Pu/Am environmental isotope assays at 106:1 (β:α) ratios; Directional-position enabled extended standoff tracking of neutron emitting (shielded/unshielded) special nuclear materials while stationary or moving at highway speeds; and, U.S. Department of Energy nuclear complex wide nuclear waste reprocessing, criticality safety, health physics, and environmental applications.

Alpha-fission-neutron spectrometry↗

Measurement of material isotopics and atom number ratio with α-particle spectroscopy for a NIFFTE fission Time Projection Chamber actinide target

In this work, we present the results of a measurement of isotopic concentrations and atomic number ratio of a double-sided actinide target using α-spectroscopy and mass spectrometry. The double-sided actinide target, with predominantly 239 Pu on one side and 235 U on the other, was used in the fission Time Projection Chamber (fissionTPC) for a measurement of the neutron-induced fission cross-section ratio between the two isotopes. The measured atomic number ratio is needed to extract an absolute measurement fission cross-section ratio. The 239 Pu/ 235 U atom number ratio was measured with a combination of mass spectrometry and α-spectroscopy with a planar silicon detector achieving uncertainties of less than 1%. Different strategies for estimating isotopic concentration from the α-spectrum are presented to demonstrate the potential of these methods for non-destructive target assay. We found that a combination of fitting spectra with constraints from mass spectrometry, and summing counts in a region of the spectrum provided the most consistent results with the lowest uncertainty.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Flash NanoPrecipitation as an Agrochemical Nanocarrier Formulation Platform: Phloem Uptake and Translocation after Foliar Administration

The increasing severity of pathogenic and environmental stressors that negatively affect plant health has led to interest in developing next-generation agrochemical delivery systems capable of precisely transporting active agents to specific sites within plants. In this work, we adapt Flash NanoPrecipitation (FNP), a scalable nanocarrier (NC) formulation technology used in the pharmaceutical industry, to prepare organic core–shell NCs and study their efficacy as foliar or root delivery vehicles. NCs ranging in diameter from 55 to 200 nm, with surface zeta potentials from -40 to +40 mV, and with seven different shell material properties were prepared and studied. Shell materials included synthetic polymers poly(acrylic acid), poly(ethylene glycol), and poly(2-(dimethylamino)ethyl methacrylate), naturally occurring compounds fish gelatin and soybean lecithin, and semisynthetic hydroxypropyl methylcellulose acetate succinate (HPMCAS). NC cores contained a gadolinium tracer for tracking by mass spectrometry, a fluorescent dye for tracking by confocal microscopy, and model hydrophobic compounds (alpha tocopherol acetate and polystyrene) that could be replaced by agrochemical payloads in subsequent applications. After foliar application onto tomato plants with Silwet L-77 surfactant, internalization efficiencies of up to 85% and NC translocation efficiencies of up to 32% were observed. Significant NC trafficking to the stem and roots suggests a high degree of phloem loading for some of these formulations. Results were corroborated by confocal microscopy and synchrotron X-ray fluorescence mapping. NCs stabilized by cellulosic HPMCAS exhibited the highest degree of translocation, followed by formulations with a significant surface charge. The results from this work indicate that biocompatible materials like HPMCAS are promising agrochemical delivery vehicles in an industrially viable pharmaceutical nanoformulation process (FNP) and shed light on the optimal properties of organic NCs for efficient foliar uptake, translocation, and delivery.

36 MATERIALS SCIENCE↗

Radioisotope dating of nuclear materials using cryogenic decay energy spectrometry

Cryogenic decay energy spectrometry provides high energy resolution and enables absolute decay counting, offering an alternative measurement technique for radiochronometry. A cryogenic decay energy spectrometry experiment was conducted using a magnetic microcalorimeter to determine the age of a plutonium sample. The energy resolution was measured at 0.05% from 5 to 6 MeV. The time since sample purification was determined using the measured concentration ratio of the 241 Am/ 241 Pu radiochronometer. Sample age estimates based on 241 Pu alpha-decay and beta-decay counts, along with 241 Am decay counts, align with the expected sample age within expanded uncertainty (k = 2), supporting the accuracy of cryogenic decay energy spectrometry as a radiochronometric method.

and nuclear chemistry↗

Erratum to: The LUX-ZEPLIN (LZ) radioactivity and cleanliness control programs

LUX-ZEPLIN (LZ) is a second-generation direct dark matter experiment with spin-independent WIMP-nucleon scattering sensitivity above 1.4 × 10 -48 cm 2 for a WIMP mass of 40 GeV/c 2 and a 1000 d exposure. LZ achieves this sensitivity through a combination of a large 5.6 t fiducial volume, active inner and outer veto systems, and radio-pure construction using materials with inherently low radioactivity content. The LZ collaboration performed an extensive radioassay campaign over a period of six years to inform material selection for construction and provide an input to the experimental background model against which any possible signal excess may be evaluated. The campaign and its results are described in this paper. We present assays of dust and radon daughters depositing on the surface of components as well as cleanliness controls necessary to maintain background expectations through detector construction and assembly. Finally, examples from the campaign to highlight fixed contaminant radioassays for the LZ photomultiplier tubes, quality control and quality assurance procedures through fabrication, radon emanation measurements of major sub-systems, and be spoke detector systems to assay scintillator are presented.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Effects of Microbial-Mineral Interactions on Organic Carbon Stabilization in a Ponderosa Pine Root Zone: A Micro-Scale Approach

Soil microbial communities affect the formation of micro-scale mineral-associated organic matter (MAOM) where complex processes, including adhesion, aggregate formation, microbial mineral weathering and soil organic matter stabilization occur in a narrow zone of large biogeochemical gradients. Here we designed a field study to examine carbon stabilization mechanisms by using in-growth mesh bags containing biotite that were placed in a ponderosa pine root zone for 6 months and compared to the surrounding bulk soil. We sought to determine the composition of the microbial community in the mesh bags compared to the surrounding soils, analyze the direct interactions between microbes and biotite, and finally identify the nature of the newly formed MAOM within the mesh-bags. Our results revealed that minerals in the mesh bags were colonized by a microbial community that produced organic matter in situ. The 16S rRNA gene sequencing and ITS2 region characterization showed phylogenetic similarity between the mesh bag and bulk soil archaea/bacteria and fungi microbiomes, with significant differences in alpha- and beta-diversity and species abundances. Organic matter pools in the mesh bags, analyzed by Fourier transform ion cyclotron resonance mass spectrometry, contained protein- (peptides) and lipid-like compounds while the bulk soil OM was comprised of lignin-like and carboxyl-rich alicyclic molecules. These results support that the newly formed biotite associated organic compounds have a microbial signature in the mesh bags. High-resolution electron microscopy documented strongly adhered organic compounds to biotite surfaces, formation of microaggregates, elemental uptake at the microbe (organic matter)-mineral interface, and distortion of biotite layers. Overall, this study shows the direct and indirect involvement of soil microbial communities from the root zone of ponderosa pine in the formation of MAOM, soil organic carbon stabilization, microaggregation, and mineral weathering at micro- and nano-scales.

58 GEOSCIENCES↗

Study of the Synchrotron Photoionization Oxidation of Alpha-Angelica Lactone (AAL) Initiated by O( 3 P) at 298, 550, and 700 K

In recent years, biofuels have been receiving significant attention because of their potential for decreasing carbon emissions and providing a long-term renewable solution to unsustainable fossil fuels. Currently, lactones are some of the alternatives being produced. Many lactones occur in a range of natural substances and have many advantages over bioethanol. In this study, the oxidation of alpha-angelica lactone initiated by ground-state atomic oxygen, O( 3 P), was studied at 298, 550, and 700 K using synchrotron radiation coupled with multiplexed photoionization mass spectrometry at the Lawrence Berkeley National Lab (LBNL). Photoionization spectra and kinetic time traces were measured to identify the primary products. Ketene, acetaldehyde, methyl vinyl ketone, methylglyoxal, dimethyl glyoxal, and 5-methyl-2,4-furandione were characterized as major reaction products, with ketene being the most abundant at all three temperatures. Possible reaction pathways for the formation of the observed primary products were computed using the CBS–QB3 composite method.

09 BIOMASS FUELS↗

Absorber Clamp for Microcalorimeter Decay Energy Spectrometry

Microcalorimeter Decay Energy Spectrometry (DES) is of interest to nuclear safeguards due to its ability to provide high precision isotopic compositions of nanogram-to microgram-scale samples of Pu and U and related daughter products. The DES method is able to record decay energy of each alpha-decay event in a sample that is embedded in a metal matrix (absorber) and thermally linked to a microcalorimeter detector. This work optimizes the DES technique used to thermally link the absorber and microcalorimeter detector element to allow for more rapid assembly and to increase detector performance and operating life. Optimized attachment methods are crucial for enhancing the viability of DES in high-sample-throughput facilities, such as those that support international nuclear safeguards measurements. Here, in this study, we designed and implemented a pressure-based absorber clamp and evaluated the performance of this new attachment method relative to pressed indium bond attachment. Results using the absorber clamp demonstrate a streamlined detector assembly procedure that minimizes accidental damage to detectors, as well as increasing detector pulse speeds by 57%. Spectral comparison shows the clamp preserves detector performance relative to indium attachment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

In situ calibration of charged particle spectrometers on the OMEGA Laser Facility using 241 Am and 226 Ra sources

Charged particle spectrometry is a critical diagnostic to study inertial-confinement-fusion plasmas and high energy density plasmas. The OMEGA Laser Facility has two fixed magnetic charged particle spectrometers (CPSs) to measure MeV-ions. In situ calibration of these spectrometers was carried out using 241 Am and 226 Ra alpha emitters. The alpha emission spectrum from the sources was measured independently using surface-barrier detectors (SBDs). The energy dispersion and broadening of the CPS systems were determined by comparing the CPS measured alpha spectrum to that of the SBD. The calibration method significantly constrains the energy dispersion, which was previously obtained through the measurement of charged particle fusion products. Overall, a small shift of 100 keV was observed between previous and the calibration done in this work.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Uniform Whole Wafer Anisotropic Etching of Structural Ta Thin Films

Tantalum (Ta) has promise as a structural material for micromechanical sensors and actuators. Anisotropic etching of alpha (α) phase Ta is required for micromachining applications. Uniform thickness and etch across a full wafer are desirable features. An experimental investigation is conducted to study plasma etching rate and anisotropy in etching α -Ta in relation to pressure and gas flow ratio. A comparatively low toxicity gas, carbon tetrafluoride (CF4), and argon (Ar) are used. Spectrometry by optical emission spectrometry (OES) and residual gas analysis (RGA) are employed to characterize the plasma to gain insight into the etch mechanisms. At low flow, the etch rate is slow due to an inadequate supply of the etching gas, CF4. The etch rate is also slowed at high flow due to a reduced CF4 residence time. Flow and pressure conditions to achieve a good etch rate and vertical sidewalls are identified and explained by means of a full factorial experiment coupled with emission spectra. Finally, with these conditions, uniform etching of 2.5 μm thick α-Ta across a 4-inch wafer is demonstrated.

36 MATERIALS SCIENCE↗

Challenges in integrating dissolved organic matter chemodiversity into kinetic models of soil respiration

The chemodiversity of dissolved organic matter (DOM) in soil has been proposed to influence the microbial metabolism and fate of belowground organic carbon (C). However, integrating DOM chemistry into soil C cycle models to improve predictions of C stocks and fluxes—beyond simply considering DOM pool size—remains a challenge. While recent research suggests that incorporating DOM chemodiversity into models can improve predictions of microbial respiration, there is still a lack of mechanistic understanding describing how DOM chemodiversity affects microbial metabolism and soil respiration. Here, we evaluated whether DOM chemodiversity was a determinant of soil respiration using paired measurements of high-resolution DOM chemistry, obtained from Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS), and potential soil respiration rates from across the United States (U.S.), all data provided by the Molecular Observation Network. Our objectives were to (1) assess statistical relationships between DOM chemodiversity and microbial respiration, and (2) evaluate the ability of kinetic models to leverage DOM chemistry to explain empirical relationships found in statistical models. Statistical regressions revealed that DOM chemodiversity (alpha diversity) was nonlinearly related to potential soil respiration rates, both independently and through its interactions with DOM and total C concentrations. In soils with relatively high DOM but low total C concentrations, potential soil respiration rates were negatively correlated with DOM alpha diversity, whereas in soils with relatively low DOM and high total C concentrations showed the opposite trend. However, when metabolic transition theory kinetic models were modified to include chemodiversity, their performance was comparable to traditional Monod kinetics approaches, which simulate respiration rates as a function of DOM concentration. The inability to account for nonlinearities in DOM chemodiversity–respiration relationships highlight an opportunity to advance substrate uptake kinetics by establishing causal links between DOM chemodiversity, microbial metabolism trade-offs, and potential interactions under varied environmental conditions.

Bioenergetic model↗

Root-associated bacterial communities and root metabolite composition are linked to nitrogen use efficiency in sorghum

ABSTRACT The development of cereal crops with high nitrogen use efficiency (NUE) is a priority for worldwide agriculture. In addition to conventional plant breeding and genetic engineering, the use of the plant microbiome offers another approach to improving crop NUE. To gain insight into the bacterial communities associated with sorghum lines that differ in NUE, a field experiment was designed comparing 24 diverse Sorghum bicolor lines under sufficient and deficient nitrogen (N). Amplicon sequencing and untargeted gas chromatography–mass spectrometry were used to characterize the bacterial communities and the root metabolome associated with sorghum genotypes varying in sensitivity to low N. We demonstrated that N stress and sorghum type (energy, sweet, and grain sorghum) significantly impacted the root-associated bacterial communities and root metabolite composition of sorghum. We found a positive correlation between sorghum NUE and bacterial richness and diversity in the rhizosphere. The greater alpha diversity in high NUE lines was associated with the decreased abundance of a dominant bacterial taxon, Pseudomonas . Multiple strong correlations were detected between root metabolites and rhizosphere bacterial communities in response to low N stress. This indicates that the shift in the sorghum microbiome due to low N is associated with the root metabolites of the host plant. Taken together, our findings suggest that host genetic regulation of root metabolites plays a role in defining the root-associated microbiome of sorghum genotypes differing in NUE and tolerance to low N stress. IMPORTANCE The development of crops that are more nitrogen use-efficient (NUE) is critical for the future of the enhanced sustainability of agriculture worldwide. This objective has been pursued mainly through plant breeding and plant molecular engineering, but these approaches have had only limited success. Therefore, a different strategy that leverages soil microbes needs to be fully explored because it is known that soil microbes improve plant growth through multiple mechanisms. To design approaches that use the soil microbiome to increase NUE, it will first be essential to understand the relationship among soil microbes, root metabolites, and crop productivity. Using this approach, we demonstrated that certain key metabolites and specific microbes are associated with high and low sorghum NUE in a field study. This important information provides a new path forward for developing crop genotypes that have increased NUE through the positive contribution of soil microbes.

59 BASIC BIOLOGICAL SCIENCES↗

Integrated Transcriptomic and Proteomic Analysis Identifies Plasma Biomarkers of Hepatocellular Failure in Alcohol-Associated Hepatitis

Alcohol-associated hepatitis (AH) is a form of liver failure with high short-term mortality. Recent results have shown that HNF4a defective function and systemic inflammation are major disease drivers of AH. Plasma biomarkers of hepatocyte function could be useful for diagnostic and prognostic purposes. Herein an integrative analysis of hepatic RNAseq and liquid chromatography-tandem mass spectrometry (LC-MS/MS) was performed to identify plasma protein signatures for mild and severe AH patients. Alcohol-related liver disease cirrhosis (ALD)(AC), non-alcoholic fatty liver disease (NALFD), and healthy subjects (HC) were used as comparator groups. Identified proteins primarily involved in hepatocellular function were decreased in AH patients which included hepatokines, clotting factors, complement cascade components, and hepatocyte growth activators. A protein signature of AH disease severity was identified including thrombin (THRB), hepatocyte growth factor alpha (HGFA), clusterin (CLUS), human serum factor H-related protein (FHR1) and kallistatin (KAIN), which exhibited large abundance shifts between severe and non-severe AH. The combination of THRB and HGFA discriminated between severe and non-severe AH with high sensitivity and specificity. These findings were correlated with the liver expression of genes encoding secreted proteins in a similar cohort, finding a highly consistent plasma protein signature reflecting HNF4A and HNF1A functions. This unbiased proteomic-transcriptome analysis identified plasma protein signatures and pathways associated with disease severity, reflecting HNF4A/1A activity useful for diagnostic assessment in AH.

60 APPLIED LIFE SCIENCES↗

Conformer-Dependent Chemistry: Experimental Product Branching of the Vinyl Alcohol + OH + O 2 Reaction

The concentration of formic acid in Earth's tropo-sphere is underestimated by detailed chemical models compared to field observations. Phototautomerization of acetaldehyde to its less stable tautomer vinyl alcohol, followed by the OH-initiated oxidation of vinyl alcohol, has been proposed as a missing source of formic acid that improves the agreement between models and field measurements. Theoretical investigations of the OH + vinyl alcohol reaction in excess O 2 conclude that OH addition to the alpha carbon of vinyl alcohol produces formaldehyde + formic acid + OH, whereas OH addition to the β site leads to glycoaldehyde + HO 2 . Furthermore, these studies predict that the conformeric structure of vinyl alcohol controls the reaction pathway, with the anti-conformer of vinyl alcohol promoting α OH addition, whereas the syn-conformer promotes β addition. However, the two theoretical studies reach different conclusions regarding which set of products dominate. We studied this reaction using time-resolved multiplexed photoionization mass spectrometry to quantify the product branching fractions. Our results, supported by a detailed kinetic model, conclude that the glycoaldehyde product channel (arising mostly from syn-vinyl alcohol) dominates over formic acid production with a 3.6:1.0 branching ratio. Additionally, this result supports the conclusion of Lei et al. that conformer-dependent hydrogen bonding at the transition state for OH-addition controls the reaction outcome. As a result, tropospheric oxidation of vinyl alcohol creates less formic acid than recently thought, increasing again the discrepancy between models and field observations of Earth's formic acid budget.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗