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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

In the nuclear explosion monitoring context, what is an anomaly?

Abstract In the early years of nuclear explosion monitoring, experts used downwind detections with meaningful ratios of radioactive species to identify an explosion. Today’s reality is sparse networks of radionuclide monitoring stations looking for weak signals. Analysts need to discriminate between industrial background radioactivity and nuclear explosion signals, even using the detection of one isotope. Aerosol and xenon measurements potentially related to nuclear tests in 2006 and 2013 announced by the Democratic People’s Republic of Korea and from worldwide civilian background radioactivity are considered when defining radionuclide detection anomalies to objectively guide the use of limited analyst resources and reduce the possibility of not detecting nuclear explosions.

Miley, Harry S.↗
NASA NTRS1986

Resonance ionization mass spectrometry for isotopic abundance measurements

Resonance ionization mass spectrometry (RIMS) is a relatively new laser-based technique for the determination of isotopic abundances. The resonance ionization process depends upon the stepwise absorption of photons from the laser, promoting atoms of the element of interest through progressively higher electronic states until an ion is formed. Sensitivity arises from the efficiency of the resonant absorption process when coupled with the power available from commercial laser sources. Selectivity derives naturally from the distinct electronic structure of different elements. This isobaric discrimination has provided the major impetus for development of the technique. Resonance ionization mass spectrometry was used for analysis of the isotopic abundances of the rare earth lutetium. Isobaric interferences from ytterbium severely effect the ability to measure small amounts of the neutron-deficient Lu isotopes by conventional mass spectrometric techniques. Resonance ionization for lutetium is performed using a continuous-wave laser operating at 452 nm, through a sequential two-photon process, with one photon exciting the intermediate resonance and the second photon causing ionization. Ion yields for microgram-sized quantities of lutetium lie between 10(6) and 10(7) ions per second, at overall ionization efficiencies approaching 10(-4). Discrimination factors against ytterbium greater than 10(6) have been measured. Resonance ionization for technetium is also being explored, again in response to an isobaric interference, molybdenum. Because of the relatively high ionization potential for Tc, three-photon, two-color RIMS processes are being developed.

Miller, C. M.↗
DOE OSTI2023

Position-specific carbon isotopes of Murchison amino acids elucidate extraterrestrial abiotic organic synthesis networks

The Murchison meteorite is a well-studied carbonaceous chondrite with relatively high concentrations of amino acids thought to be endogenous to the meteorite, in part because they are characterized by carbon isotope (δ 13 C) values higher than those typical of terrestrial amino acids. Past studies have proposed that extraterrestrial amino acids in the Murchison meteorite could have formed by Strecker synthesis (for α-amino acids), Michael addition (for β-amino acids), or reductive amination, but a lack of constraints have prevented confident discrimination among these possibilities, or assignment of specific formation pathways to each of several specific amino acids. Position-specific carbon isotope analysis differentiates amongst these mechanisms by relating molecular sites to isotopically distinct carbon sources and by constraining isotope effects associated with elementary chemical reactions. Prior measurements of the position-specific carbon isotopic composition of α-alanine from the Murchison CM chondrite demonstrated that alanine’s high δ 13 C VPDB value is attributable to the amine carbon (δ 13 C VPDB = +142 ± 20‰), consistent with Strecker synthesis drawing on 13 C-rich carbonyl groups in precursors (Chimiak et al., 2021). Here, we measured the δ 13 C composition of fragment ions generated by electron impact ionization of derivatized α-alanine, β-alanine, and aspartic acid from Murchison via gas chromatography-Fourier transform mass spectrometry. α-Alanine’s amine carbon yielded δ 13 C VPDB = +109 ± 21‰, which is consistent with the previously measured value and with formation from 13 C-rich precursors. β-Alanine’s amine carbon presents a lower δ 13 C VPDB = +33 ± 24‰, which supports formation from 13 C-rich precursors but potentially via a Michael addition mechanism rather than Strecker synthesis. Aspartic acid’s amine carbon has δ 13 C VPDB = -14 ± 5‰, suggesting synthesis from precursors distinct from those that generated the alanine isomers. Further, these measurements indicate that Murchison amino acids are a mixture of compounds made from different synthesis mechanisms, though some subsets likely drew on the same substrates; this conclusion highlights the complexity of extraterrestrial organic synthesis networks and the potential of emerging methods of isotope ratio analysis to elucidate the details of those networks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

A PIPS + SrI 2 (Eu) detector for atmospheric radioxenon monitoring

The PIPS–SrI 2 (Eu) is a prototype atmospheric radioxenon detection system designed at Oregon State University in support of international efforts towards monitoring clandestine nuclear weapon testing activities. This detector aims to address some shortcomings found in currently deployed beta–gamma atmospheric radioxenon detection systems, such as lackluster energy resolution and memory effect, by employing modern detection materials and readout. The system uses a PIPSBox, a silicon-based gas cell, for electron detection, and a pair of ultrabright, D-shaped SrI 2 (Eu) scintillators coupled to silicon photomultipliers for photon detection. A custom eight-channel digital pulse processor equipped with a field programmable gate-array (FPGA) identifies electron–photon coincidences between the volumes in near real-time. Gas samples of the four radioxenon isotopes of interest were independently measured with the PIPS–SrI 2 (Eu) detection system to determine energy resolution and efficiency. Application of FPGA-based coincidence discrimination in near real-time reduced the ambient background count rate by 95.85 ± 0.04%. Using parameters from the Xenon International gas processing unit and assuming a blank sample and zero memory effect the minimum detectable concentrations (MDCs) for the isotopes were calculated to be 0.12 ± 0.03, 0.27 ± 0.05, 0.15 ± 0.02, and 1.00 ± 0.08 mBq/m 3 air for 131m Xe, 133 Xe, 133m Xe, and 135 Xe, respectively. These MDC estimates compare well with other radioxenon detection systems employed in the International Monitoring System (IMS) and indicate that the PIPS–SrI 2 (Eu) is in compliance with the Comprehensive Nuclear Test-Ban-Treaty Organization (CTBTO) sensitivity requirement of ≤ 1 mBq/m 3 for 133 Xe.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Isotope effects at the origin of life: Fingerprints of the Strecker synthesis

We report strecker synthesis creates α-amino acids from prebiotically plausible substrates (cyanide, ammonia, and aldehydes) and is widely hypothesized to be a key mechanism in the chemistry that led to life on Earth and on other planets. To better constrain the synthetic environments and precursors of abiotic α-amino acids, and to determine unique signatures of abiogenic amino acids, we measured the molecular-averaged and site-specific carbon and nitrogen isotope effects for the Strecker synthesis of alanine. The reaction steps of the Strecker synthesis can be divided into two groups: an initial series of reversible amination and nitrile-addition reactions (‘equilibration’) and a second series of irreversible hydrolysis reactions (‘hydrolysis’). The equilibration of cyanide, acetaldehyde, and ammonia with the intermediate, α-aminopropionitrile (α-APN), has a measured 55.1‰ equilibrium nitrogen isotope effect between the 15 N-rich amine nitrogen in α-aminopropionitrile and the 15 N-poor ammonia and a 20.0‰ equilibrium carbon isotope effect between the 13 C-poor C-2 site in α-aminopropionitrile and the 13 C-rich carbonyl carbon in acetaldehyde. The first irreversible hydrolysis step is inferred to have an up to 10‰ normal carbon fractionation (i.e., faster for 12 C, slower for 13 C) for the whole molecule, but it also has one or more side reactions that deplete the reactive α-APN reservoir by up to 15‰. The second hydrolysis step has a 15.4‰ normal kinetic isotope effect on the amide (C-1) site of alaninamide, which becomes the carboxyl site of alanine. Other α-amino acids will likely experience similar nitrogen isotope fractionations between ammonia and their amine sites, and similar carbon isotope fractionations between the carbonyl carbon in reactant aldehydes or ketones and the intermediate α-aminonitrile, and between cyanide and the carboxyl site. Therefore, these isotope effects allow us to predict the carbon and nitrogen isotopic contents and intramolecular structures of α-amino acids formed by Strecker synthesis based on their substrates’ isotopic compositions, or to infer the isotopic compositions of substrates from which amino acids formed, for example in the case of the amino-acid-rich carbonaceous chondrites. The site-specific C and N isotopic compositions of amino acids formed by Strecker chemistry contrast with those typical of terrestrial biosynthetic amino acids, so these data also provide a means of discriminating between biogenic and abiogenic α-amino acids.

58 GEOSCIENCES↗
NASA NTRS2019

Elemental Variation and Petrogenesis of Pyroxenes in HED Meteorites by Multivariable Discriminant Analysis Method

HED (Howardite, Eucrite and Diogenite) are meteorites with mafic and ultramafic igneous composition. Previous studies suggested HED came from asteroid (4) Vesta and they were generated by magmatic melting followed by differentiation crystallization, metamorphic, and impact. Uniform oxygen isotopic composition of HED samples favors global magma ocean for (4) Vesta. However, the petrological diversity of HED may indicate more complex magma processes in the meteorites. In general, most of the geochemical studies are using traditional methods (e.g. element to element or ratio to ratio plots) to classify the different rock type and groups. With the traditional methods, only limited elements can be shown in a figure. As such, some meteorites may have been identified as HED by a traditional method but found different either in isotopic composition or other elemental characteristic. These anomalous HED meteorites may or may not come from asteroid (4) Vesta. In fact, magma is a unit system where any elemental change should affect to all other elements as a whole, it would be reasonable to consider all elements together to look for the systematical changes. Using multivariable discriminant analysis (MDA) method is one of such testing for their geochemical variation. The method may be able to help us to better understand the petrologic processes and the relationship among elements. This study is to test the MDA method by focus mainly on pyroxene composition of eucrite and diogenite.

Peng, Z. X.↗
DOE OSTI2023

Short-lived noble gas effluent trends from a research reactor

An understanding of anthropogenic sources of radioactive noble gases in the atmosphere is needed to enhance the discrimination ability of the International Monitoring System's sensors. These sources include commercial and research nuclear reactors and medical isotope production facilities. While abiding by local environmental ordinances these facilities all emit noble gas radioisotopes through normal operation. Here, this research presents measurements and analysis of noble gas isotopes ( 41 Ar, 135 Xe, 135m Xe, 137 Xe, 138 Xe, 87 Kr, 88 Kr, and 89 Kr) made directly at the stack of the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory. The Xe and Kr noble gases are concurrently observed with 41 Ar, a neutron activation product, when the reactor is operational. The magnitude of the Xe and Kr noble gases released is not constant over the HFIR cycle, but they temporally match the 41 Ar trend. An isotope activity ratio analysis of these shorter lived isotopes combined with the observation of the cycle's temporal trend helps understand the noble gas production mechanism at the HFIR. Isotopes with short half-lives are not useful for long-range environmental monitoring. However, these measurements could potentially be combined with atmospheric modeling to predict the background source term of the longer-lived Xe ratios at a monitoring station.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRS1986

The reality of the secular change in solar wind nitrogen isotopes

Evidence concerning the isotopic composition of N in the early solar system currently seems to favor a picture of isotopic inhomogeneity rather than of a unique primordial composition modified by local processes. Certainly the range of N-15/N-14 ratios found in meteorites points to the existence of more than one nucleogenetic N component, though mass dependent modification of them explain the isotopic variation observed for N in the lunar regolith. The observational evidence is addressed which can be used to discriminate between such a model and one invoking a secular change in the composition of the solar wind. Three tests of this model were considered, starting with a search for light planetary N surviving in lunar rocks. Results so far are negative. The results of these tests may not eliminate the two component model for regolith N but they seriously weaken it. The alternate view, involving a secular change in solar wind N composition, has its problems but continues to survive by default.

Kerridge, J. F.↗
DOE OSTI2021

Seasonal and Interspecific Variation in Frugivory by a Mixed Resident-Migrant Overwintering Songbird Community

Many temperate passerine bird species switch from diets of mostly invertebrates in the spring and summer to diets that include fruit and seeds in the fall and winter. However, relatively few studies have quantified diet composition or the extent of seasonal shifts during the non-breeding period, particularly among species and across communities with both residents and migrants. We measured carbon and nitrogen stable isotope values in food items (fruits, C3 and C4 seeds, and insects from various trophic levels and plant communities) and in multiple tissues (feathers and plasma/whole blood) from 11 species of songbirds wintering in the southeastern U.S. We combined these diet and tissue values with empirically derived discrimination factors and used concentration-dependent mixing models to quantify seasonal diet shifts. We also validated mixing model results with data from fecal samples. Diets in this bird community, as delineated N and C isotopic space, diverged in the fall and winter relative to the summer as consumption of fruits and seeds increased. Across this songbird community, estimated contributions of fruit to plasma/whole blood increased from 16.2 ± 7.5% in the fall (mean ± SD; range: 4–26%) to 21.7 ± 10.3% (range: 9–37%) in the winter, while contributions of seeds increased from 29.4 ± 2.6% (range: 28–32%) in the fall to 36.6 ± 4.8% (range: 32–42%) in the winter. Fecal data showed qualitatively similar trends to mixing models, but consistently estimated higher contributions of fruit. Our work indicates that fruits and seeds constitute substantial sources of sustenance for non-breeding songbirds, there is considerable separation of resource use among species in the fall and winter, and fecal estimates of contributions to songbird tissues should be interpreted cautiously.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Structural Polymorphism of Chitin and Chitosan in Fungal Cell Walls From Solid-State NMR and Principal Component Analysis

Chitin is a major carbohydrate component of the fungal cell wall and a promising target for novel antifungal agents. However, it is technically challenging to characterize the structure of this polymer in native cell walls. Here, we recorded and compared 13 C chemical shifts of chitin using isotopically enriched cells of six Aspergillus, Rhizopus, and Candida strains, with data interpretation assisted by principal component analysis (PCA) and linear discriminant analysis (LDA) methods. The structure of chitin is found to be intrinsically heterogeneous, with peak multiplicity detected in each sample and distinct fingerprints observed across fungal species. Fungal chitin exhibits partial similarity to the model structures of α- and γ-allomorphs; therefore, chitin structure is not significantly affected by interactions with other cell wall components. Addition of antifungal drugs and salts did not significantly perturb the chemical shifts, revealing the structural resistance of chitin to external stress. In addition, the structure of the deacetylated form, chitosan, was found to resemble a relaxed two-fold helix conformation. This study provides high-resolution information on the structure of chitin and chitosan in their cellular contexts. The method is applicable to the analysis of other complex carbohydrates and polymer composites.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Prototype reactor-antineutrino detector based on 6 Li-doped pulse-shape-discriminating plastic scintillator

An aboveground 60-kg reactor-antineutrino detector prototype, comprising a two-dimensional array of 36 6 ⁢Li-doped pulse-shape-sensitive plastic scintillator bars, is described. Each bar is 50 cm long with a square cross section of 5.5 cm. Doped with 6 ⁢Li at 0.1% by mass, the detector is capable of identifying correlated energy depositions for the detection of reactor antineutrinos via the inverse-𝛽-decay (IDB) reaction. Each bar is wrapped with a specular reflector that directs photons toward photomultiplier tubes mounted at both ends of the bar. Here, this paper highlights the construction, key features, and main performance characteristics of the system. The system, which relies on multiple observables such as pulse-shape discrimination, energy, position, and timing, is capable of detecting IBD-like neutron-correlated backgrounds, long-lived decay chains, and cosmogenic isotopes.

Physics↗
DOE OSTI2022

CUPID: The Next-Generation Neutrinoless Double Beta Decay Experiment

We report CUPID is a next-generation tonne-scale bolometric neutrinoless double beta decay experiment that will probe the Majorana nature of neutrinos and discover lepton number violation in case of observation of this singular process. CUPID will be built on experience, expertise and lessons learned in CUORE and will be installed in the current CUORE infra-structure in the Gran Sasso underground laboratory. The CUPID detector technology, successfully tested in the CUPID-Mo experiment, is based on scintillating bolometers of Li 2 MoO 4 enriched in the isotope of interest 100 Mo. In order to achieve its ambitious science goals, the CUPID collaboration aims to reduce the backgrounds in the region of interest by a factor 100 with respect to CUORE. This performance will be achieved by introducing the high efficient α/β discrimination demonstrated by the CUPID-0 and CUPID-Mo experiments, and using a high transition energy double beta decay nucleus such as 100 Mo to minimize the impact of the gamma background. CUPID will consist of about 1500 hybrid heat-light detectors for a total isotope mass of 250 kg. The CUPID scientific reach is supported by a detailed and safe background model based on CUORE, CUPID-Mo and CUPID-0 results. The required performances have already been demonstrated and will be presented.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS2014

In Situ Probe Science at Saturn

A fundamental goal of solar system exploration is to understand the origin of the solar sys-tem, the initial stages, conditions, and processes by which the solar system formed, how the formation pro-cess was initiated, and the nature of the interstellar seed material from which the solar system was born. Key to understanding solar system formation and subsequent dynamical and chemical evolution is the origin and evolution of the giant planets and their atmospheres. Several theories have been put forward to explain the process of solar system formation, and the origin and evolution of the giant planets and their atmospheres. Each theory offers quantifiable predictions of the abundances of noble gases He, Ne, Ar, Kr, and Xe, and abundances of key isotopic ratios 4He3He, DH, 15N14N, 18O16O, and 13C12C. Detection of certain dis-equilibrium species, diagnostic of deeper internal pro-cesses and dynamics of the atmosphere, would also help discriminate between competing theories. Measurements of the critical abundance profiles of these key constituents into the deeper well-mixed at-mosphere must be complemented by measurements of the profiles of atmospheric structure and dynamics at high vertical resolution and also require in situ explora-tion. The atmospheres of the giant planets can also serve as laboratories to better understand the atmospheric chem-istries, dynamics, processes, and climates on all planets including Earth, and offer a context and provide a ground truth for exoplanets and exoplanetary systems. Additionally, Giant planets have long been thought to play a critical role in the development of potentially habitable planetary systems. In the context of giant planet science provided by the Galileo, Juno, and Cassini missions to Jupiter and Sat-urn, a small, relatively shallow Saturn probe capable of measuring abundances and isotopic ratios of key at-mospheric constituents, and atmospheric structure in-cluding pressures, temperatures, dynamics, and cloud locations and properties not accessible by remote sens-ing can serve to test competing theories of solar system and giant planet origin, chemical, and dynamical evolution.

Interstellar↗
DOE OSTI2025

Characterization of Neutron Emission Rates of Commercial 252 Cf Sources

Accurate knowledge of 252 Cf neutron emission rates is critical for modeling and fast-neutron experiments, yet commercial sources are often supplied without traceable calibration or uncertainty estimates. This report describes a method to characterize 252 Cf sources using a pulse-shape-discrimination (PSD) scintillator. The scintillator was efficiency-calibrated against a time-tagged 252 Cf fission chamber manufactured at ORNL over 40 years ago. Isotopic evolution of the calibration source was modeled using Bateman equations to account for changes in the effective average neutrons per fission at the time of measurement. The calibrated scintillator was then used to measure absolute emission rates of several commercial 252 Cf sources, revealing deviations of up to 12% from nominal manufacturer values. This methodology provides a practical approach for establishing uncertainty-quantified 252 Cf neutron emission rates, improving fidelity in simulations and supporting the accurate interpretation of measurements.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗
NASA NTRS2020

Identification of Anomalous Eucrites and Diogenites by Multivariable Discriminant Analysis

Howardite, eucrite and diogenite clan (HED) is the largest magmatic achondrite group and has been suggested to be derived from asteroid (4) Vesta (e.g., [1]). Previous geochemical studies have suggested HEDs were generated by asteroid melting followed by crystallization, metamorphism, and impact [1-6]. However, numerous eucrites and diogenites have anomalous compositional, isotopic or petrological characteristics compared to the norm. This diversity might indicate more complex magma processes on the parent asteroid, or they could be linked to different parental asteroids (e.g., [5]). The former case would imply that the parent asteroid is more heterogenous than currently thought, and that our petrologic models are too simple. The latter case would increase the number of asteroids known to have formed mafic crusts, and would allow for petrological comparisons across numerous bodies. We apply multivariable discrimination analysis (MDA) to a large database of HED pyroxene analyses. This technique allows all elemental information to be considered simultaneously to facilitate identification of groupings, trends, and outliers within the dataset.

Peng, Z. X.↗
DOE OSTI2025

Optimizing a detection system for fissile material in nuclear disarmament verification

In arms control treaties, verification plays a crucial role in detecting non-compliance, deterring future violations, and building trust between state parties. Neutron interrogation that induces fission reactions in fissile isotopes and measures the resulting fission neutrons, could be employed for this purpose. This study aims to develop a system which can determine the presence of fissile material while intrinsically protecting information. In this paper, we focus on optimizing the system for discriminating between an enriched uranium block from a depleted uranium (DU) block. The system was built and we report on benchmark measurements with DU and 16% enriched uranium blocks. Furthermore, the Excalibur (Experiment for Calibration with Uranium) neutron source, a neutron spectrometer (redBubble Technology Industries (BTI) N-Probe), and superheated droplet detectors were used for these measurements. MCNP simulations provided insights into detector responses to fissile materials with varying isotopic compositions, confirming that the system functioned as designed.

Active neutron interrogation↗
DOE OSTI2024

Overcoming photobleaching in imaging of single barium atoms in a solid xenon matrix

Neutrinoless double beta decay is one of the most sensitive probes for new physics beyond the Standard Model of particle physics. One of the isotopes under investigation is 136 Xe, which would double beta decay into 136 Ba. Detecting the single 136 Ba daughter provides a sort of ultimate tool in the discrimination against backgrounds. Previous work demonstrated the ability to perform single atom imaging of Ba atoms in a single-vacancy site of a solid xenon matrix. In this paper, the effort to identify signal from individual barium atoms is extended to Ba atoms in a hexa-vacancy site in the matrix and is achieved despite increased photobleaching in this site. Abrupt fluorescence turn-off of a single Ba atom is also observed. Significant recovery of fluorescence signal lost through photobleaching is demonstrated upon annealing of Ba deposits in the Xe ice. Following annealing, it is observed that Ba atoms in the hexa-vacancy site exhibit antibleaching while Ba atoms in the tetra-vacancy site exhibit bleaching. This may be evidence for a matrix site transfer upon laser excitation. Our findings offer a path of continued research toward tagging of Ba daughters in all significant sites in solid xenon.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRSDate not supplied

Lunar Payloads to Constrain Exospheric Water through the NASA M-STAR program

Our understanding of water cycles on the Moon has significantly enhanced recent observations by Chang E-5, Lunar Prospector, and Chandrayaan-1 missions indicating the existence of an active water cycle on the Moon. In a new partnership between Delaware State University (DSU) and NASA Goddard Space Flight Center, enabled through the NASA’s M-STAR (MUREP Space Technology Artemis Research) program, we are developing low mass and power lunar rover payloads to enable long-duration human exploration missions. Payload technologies include wavelength modulation absorption spectroscopy to simultaneously detect water (H16OH) and isotopes (H16OD) in the (6700 nm) mid-infrared region using a closed path in compact Herriot cell optical design and wavelength modulation spectroscopy, and (2) Laser-induced breakdown spectroscopy (LIBS) to simultaneously detect and correlate water isotopes with characteristics elemental composition of lunar regolith. Due to the airless atmosphere of the Moon, we will utilize Artificial intelligence (AI) and Machine learning (ML) approaches to discriminate spectral interference with instrument drifts and correlate mid-IR trace gas profile with LIBS spectral information. This partnership will initiate a STEM engagement space program, e.g., Lander and CubeSat payload technology development for students and the next-generation NASA workforce for future lunar and Mars missions. DSU, a Historically Black University, prides itself in its proven excellence in teaching and research. It enrolls a diverse population of students (~5000) traditionally underrepresented in STEM disciplines. DSU has established itself at the forefront of optics and photonics research that transcends multidisciplinary fields of earth sciences, environmental, defense, and biomedical sensing applications.

water cycles↗