Search NASA⌕ Search

SEARCH · Search NASA

Results for “Nuclear safeguards”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

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 ↗
DOE OSTI2023

Online monitoring the hydrolysis of uranium hexafluoride for intermediates by cryogenic layering and FTIR

Uranium hexafluoride (UF 6 ) is a commonly utilized material feedstock in uranium enrichment processes due to its high vapor pressure and ease of sublimation. When exposed to air, UF 6 undergoes spontaneous hydrolysis to form uranyl fluoride (UO 2 F 2 ) particulates which are utilized for the detection of undeclared nuclear activities by nuclear safeguards organizations. In this study, the kinetics of the hydrolysis reaction and how they relate to particle morphology of the product are still debated in the literature. Here, we report the direct, in situ observation of UF 6 reaction intermediates by cooling the reaction to cryogenic temperatures to significantly reduce the rate of hydrolysis. The reaction is then observable by Fourier transform infrared (FTIR) spectroscopy. The conversion of UF 6 to UOF 4 is observed as well as several other bands associated with possible long lived intermediate complexes. Chemometrics are used to further elucidate the reaction pathway from UF 6 to UO 2 F 2 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Plutonium Basket Counter Measurement Control Q3-Q4 2023

The Plutonium Basket Counter (PBC) is a spent fuel nuclear safeguards instrument that was developed to measure spent-fuel elements from MAGNOX-type research reactors and determine their plutonium content. The instrument is designed to measure fuel elements in spent fuel cooling pools through underwater operation, but it is also able to measure radiation sources in air. The PBC determines fuel plutonium content by detecting neutrons with an array of Helium-3 detectors. The electronics make use of a JSR-15 shift register for data collection and IAEA Neutron Coincidence Counting (INCC) software for data analysis. The PBC is used to determine the 240 Pu content in spent MAGNOX fuel elements grouped into basket-like bundles, thus the instrument’s name. Reactor burnup calculations can be used in conjunction with the data from the PBC to estimate the total plutonium content in the fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Neutron and Gamma-Ray Imaging of Th-232 and Cm-244 Using Organic Glass Scintillators

Modern nuclear safeguards require detection and characterization capabilities suitable for a wide variety of radiation sources and applications. Field-deployable detection systems have also had to modernize to meet changing needs. Recent developments in organic scintillator technology have resulted in the creation of an organic glass scintillator (OGS) at Sandia National Laboratory which is composed of a 9:1 mixture of glass compounds C42H36Si and C51H44Si. The novel scintillator composition was implemented into the design for a dual-particle capable imaging system at the University of Michigan. This work presents new results from two experiments demonstrating the gamma-ray and fast-neutron imaging capabilities of the organic glass system. Gamma spectroscopy was also performed using CeBr3 scintillators that are part of the imager design. Measurements were performed at Lawrence Livermore National Laboratory using 232Th metal hemishells and an encapsulated 244Cm oxide source. Successful gamma-ray imaging of the 232Th distributed sources is demonstrated with the glass imager, but there were no appreciable neutrons from the 232Th for neutron imaging. Promising neutron and gamma-ray imaging results of 244Cm are demonstrated despite limited imaging event statistics available in this measurement. Gamma-ray spectroscopy results were able to identify 232Th using prominent emissions at 239, 338, 583, and 911 keV. 244Cm was identified from emissions of 43, 99, and 153 keV. These results demonstrate the potential of organic glass imaging for nuclear nonproliferation or characterization efforts.

Lopez, Ricardo [Univ. of Michigan, Ann Arbor, MI (↗
DOE OSTI2022

Space-dependent calculation of the multiplicity moments for shells

In earlier work, we extended the methodology of multiplicity counting in nuclear safeguards, by elaborating the one-speed stochastic transport theory of the calculation of the so-called multiplicity moments, i.e. the factorial moments of the number of neutrons emitted from a fissile item, following a source event from an internal neutron source (spontaneous fission and (α, n) reactions). Calculations were made for spheres and cylinders of various shapes. In all our work so far, the material of the items was homogeneous, and the distribution of the internal source was assumed to be uniformly distributed within the item, with the neutron emission assumed to be isotropic. In the present work the calculations are extended to the case of a point source inside either a solid sphere or in a spherical shell. This necessitates the extension of the theory to non-homogeneous items and non-uniform and non-isotropic sources. This work describes the extension of the theory and provides some quantitative results. (authors)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Application of SAMMY for Non-Destructive Characterization of Irradiated Samples Using Neutron Transmission Measurements at VENUS

This report presents the application of SAMMY (Larson 2008), an R-matrix Bayesian fitting system, for analyzing neutron transmission data to enable non-destructive isotopic identification. Transmission measurements were conducted at the VENUS (Bilheux et al. 2023) beamline of the Spallation Neutron Source (SNS) using samples with unknown or partially characterized compositions. Through the application of SAMMY’s R-matrix Bayesian fitting capabilities to the measured transmission spectra and comparison against evaluated nuclear data libraries, isotopic constituents can be quantitatively determined based on their characteristic neutron resonance signatures. This methodology demonstrates significant potential for applications in nuclear safeguards, forensics, and post-irradiation examination.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Large area position sensitive detector for thermal neutrons

Large area thermal neutron detectors are applied in many fields including industrial imaging, nuclear safeguarding, neutron scattering, and fundamental science. Historically, these detectors were based on 3 He gas proportional counters despite the limitations of 3 He detectors such as high cost, limited supply, non-uniform spatial resolution, and depth of absorption problems. Two alternatives to 3 He detectors are 6 Li-loaded glass scintillators, and powdered ZnS(Ag) scintillators mixed with 6LiF neutron converters. The 6 LiF/ZnS(Ag) scintillator has advantages over 6 Li glass as it is less expensive and can be produced in larger areas, although its self-absorption presents a problem. In this work, we developed a large area thermal neutron detector based on 6 LiF/ZnS(Ag) scintillator coupled with wavelength shifting fibers. The detector uses resistive charge divider-based position encoding. We further modified and improved the method by 2D segmentation of the detector using modular multichannel readout electronics. This segmentation approach allows for a combination of large detector area, improved spatial resolution, and increased count rate. Furthermore, spatial resolution can be variable across the detector area by adjusting the segment size.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Space-Dependent Calculation of the Multiplicity Moments for Shells With the Inclusion of Scattering

In recent work, we extended the methodology of multiplicity counting in nuclear safeguards by elaborating the one-speed stochastic transport theory of the calculation of the so-called multiplicity moments, i.e., the factorial moments of the number of neutrons emitted from a fissile item, following a source event from an internal neutron source [spontaneous fission and (α; n) reactions]. Calculations were made for solid spheres and cylinders, with the source being homogeneously distributed within the item. Recent measurements of the Rocky Flats Shells during the Measurement of Uranium Subcritical and Critical (MUSIC) campaign conducted by Los Alamos National Laboratory and assisted by the University of Michigan inspired us to extend the model to spherical shell geometry with a point source in the middle of the central cavity. Comparison of the calculated results with the experimental ones indicated that accounting for fission as the only neutron reaction (the standard procedure in the point model, adapted also in our work so far) was not sufficient for reaching good agreement with measurements. The model was therefore extended to include elastic scattering into the one speed formalism, whereas the effect of inelastic scattering was accounted for in an empirical way. After these extensions, good agreement was found between the calculated and the measured values. The paper describes the extension of the theory and provides concrete quantitative results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Matrix-Assisted Ionization of Molecular Uranium Species

Matrix-assisted ionization (MAI) demonstrates high sensitivity for a variety of organic compounds; however, few studies have reported the application of MAI for the detection and characterization of inorganic analytes. Trace-level uranium analysis is important in the realms of nuclear forensics, nuclear safeguards, and environmental monitoring. Traditional mass spectrometry methods employed in these fields require combinations of extensive laboratory chemistry sample preparation and destructive ionization methods. There has been recent interest in exploring ambient mass spectrometry methods that enable timely sample analysis and higher sensitivity than what is attainable by field-portable radiation detectors. Rapid characterization of uranium at nanogram levels is demonstrated in this study using MAI techniques. Mass spectra were collected on an atmospheric pressure mass spectrometer for solutions of uranyl nitrate, uranyl chloride, uranyl acetate, and uranyl oxalate utilizing 3-nibrobenzonitrile as the ionization matrix. The uranyl complexes investigated were detectable, and the chemical speciation was preserved. Sample analysis was accomplished in a matter of seconds, and limits of detection of 5 ng of uranyl nitrate, 10 ng of uranyl oxalate, 100 ng of uranyl chloride, and 200 ng of uranyl acetate were achieved. The observed gas-phase speciation was similar to negative-ion electrospray ionization of uranyl compounds with notable differences. Six matrix-derived ions were detected in all negative-ion mass spectra, and some of these ions formed adducts with the uranyl analyte. Subsequent analysis of the matrix suggests that these molecules are not matrix contaminants and are instead created during the ionization process.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Direct analysis of cotton swipes for plutonium isotope determination by microextraction-ICP-MS

This study demonstrates a method for determining the isotopic composition of low-level (sub-pg) plutonium (Pu) directly from a cotton swipe. Environmental sample (ES) swipes are routinely employed as a tool for monitoring activities in nuclear facilities. Traditional ES swipe analysis, as employed in nuclear safeguards, utilizes laborious ashing, digestion, and chemical separation procedures prior to mass spectrometric (MS) analysis. Here, an innovative sample introduction technique employing a microextraction probe to extract Pu directly from the swipe surface is described. The microextraction probe lowers onto the swipe surface, seals on a small area (8 mm 2 ), and delivers solvent (2% HNO 3 ) to extract actinide material that may be present. The extracted analyte is subsequently directed into a sector field inductively coupled plasma (ICP)-MS for isotope ratio determination. This microextraction-ICP-MS method successfully determined the isotopic composition ( 240 Pu/ 239 Pu and 242 Pu/ 239 Pu) of three Pu certified reference materials (CRM 136, 137, and 138) that were deposited (1 pg) onto ES swipes. The percent relative difference from the certified value, uncorrected for instrumental fractionation, was <2% for the 240 Pu/ 239 Pu ratio on all three CRMs and <10% for the 242 Pu/ 239 Pu ratio on CRM 136 and 138. Here, the percent relative standard deviation, an estimate of the sample-to-sample isotopic precision, was <4% for the 240 Pu/ 239 Pu and <15% for the 242 Pu/ 239 Pu. Method limits of detection were determined, based on measurements of an enriched 244 Pu material, to be ~7 fg. Additionally, a mixed uranium (U) and Pu deposition was made to determine the method's ability to simultaneously extract U and Pu and determine the isotopic composition of both analytes.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

Light-powered end-to-end neutron detection and imaging with an edge-deployed optical AI chip

Neutron detection is widely used in many applications including nuclear physics, nuclear energy, nuclear technologies and nuclear safeguards. Developing an end-to-end neutron detection and imaging workflow paves way towards fully automated processes for many applications. We implemented an automated workflow for neutron detection experiments which use a solid state image sensor to capture neutron hits as a digital image. We deploy the workflow to an edge-based optical neural network (ONN) to increase the radiation-hardness and lifetime of neutron detection instruments. We present a two-stage neural network framework for detection of neutrons at sub-pixel resolution. The first stage uses a region proposal network to efficiently detect and extract neutron hits from the input camera image. The second stage feeds the extracted hits into a fully connected neural network to predict the sub-pixel hit position. The performance of the two-stage framework is evaluated using the edge-based ONN. The results show that we can achieve above 96% neutron detection accuracy as well as sub-pixel and sub-micron position resolution, while enjoying the advantages of the ONN hardware including radiation-hardness, low energy consumption and high computing speed for integrated edge camera and hardware deployment, when compared with electronic counterparts.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Towards Three-Dimensional Neutron Imaging with Light-field Technology

A broad range of applications in nuclear safeguards and security can benefit from compact, fast neutron imagers with large angular acceptance. However, accurate 3D multi-vertex reconstruction in a monolithic detector remains a significant barrier to realization. Current approaches, such as the centroiding approach and the use of shadow masks, have not yet resulted in a successful demonstration in a light-starved environment. This project explored the use of cutting-edge technology—a light field camera—which inherently preserves both the spatial and directional information of incident light. Such technology can, in principle, resolve multi-vertex events and offer accurate position reconstruction in 3D with relatively simple readout electronics. Since the project's inception in May 2023, we have built an experimental setup to calibrate and characterize a commercial light-field camera (Lytro Illum). We assessed its 3D event reconstruction capability in a relatively low-light intensity environment by analyzing the cross-correlation of a series of 2D images of a characterized tunable light source taken at various distances. A sub-cm resolution, lower than typical neutron interaction separations in a compact scintillator volume, was observed with the LED light source, suggesting the promising capability of its nominal optics design to provide the adequate resolution required for a compact monolithic neutron directional detector. However, using a light-field-based readout for a neutron camera requires incorporating an ultra-low-noise light sensor, which is beyond the scope of this project. We also initiated the development of a 3D light-field-based reconstruction algorithm tailored to sparse scenes, as expected from particle interactions in a scintillator medium. Additionally, we demonstrated the capability of the algorithm to replicate the ground truth. Finally, we began the development of a neutron directional detector simulation to determine the performance criteria for light-field-based reconstruction that allows for good neutron directional reconstruction. This Feasibility Study has led to a successful follow-up project under the DNN R&D innovation portfolio starting May 2024.

42 ENGINEERING↗
DOE OSTI2022

Direct isotopic analysis of solid uranium particulates on cotton swipes by microextraction-ICP-MS

Direct isotope ratio analysis of solid uranium particulates on cotton swipes was achieved using a solution-based microextraction technique, coupled to a quadrupole inductively coupled plasma - mass spectrometer (ICP-MS). This microextraction-ICP-MS methodology provides rapid isotopic analysis which could be applicable to nuclear safeguards measurements. Particulates of uranyl nitrate hexahydrate (UO 2 (NO 3 ) 2 ·6H 2 O) and uranyl fluoride (UO 2 F 2 ) ranging from 6 μm to 40 μm in length were transferred to cotton swipes with a particle manipulator. The microextraction probe then delivers a 5% nitric acid (HNO3) solvent onto the swipe surface to extract the uranium species. The extracted sample is then delivered to the ICP-MS for isotopic determination. The majority of uranium signal (~99% and ~94% for UO2(NO3)2·6H2O and UO 2 F 2 , respectively) was detected in the first 15 s extraction, while subsequent extractions on the same location had low or no U signal, suggesting near complete removal of the solid uranium compounds from the swipe surface. Ten samples (for each of the uranium compounds), were analyzed for their isotopic composition. For UO 2 (NO 3 ) 2 ·6H 2 O, the determined isotope ratios resulted in a % relative difference (% RD) from the referenced isotope ratios of 0.97, 1.0, and 7.3% for 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U, respectively. The % RD of the UO 2 F 2 isotope ratios were 1.9 and 0.60% for 234 U/ 238 U and 235 U/ 238 U, respectively. The preliminary limits of detection were determined to be 0.002, 0.4, and 60 pg for 234 U, 235 U and 238 U, respectively This work demonstrates that microextraction ICP-MS is a rapid and sensitive method that could directly determine uranium isotope ratios of UO 2 (NO 3 ) 2 ·6H 2 O and UO 2 F 2 particulates on cotton swipes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Understanding the structural and morphological effects of synthesis route on NpO 2

The availability of actinide standard materials for use in nuclear safeguard applications is critical, as is thorough characterization thereof. Although accurate trace element compositions and isotopic considerations are paramount for deployment of reference standards, structural characterization is also essential towards accurately describing the chemical form and potential matrix effects in candidate materials. Here, to this end, samples of NpO 2 were synthesized via a direct denitration (DD) method and probed with powder X-ray diffraction (PXRD), Raman spectroscopy, and scanning electron microscopy (SEM) for structural and morphological characterization and comparison with NpO 2 materials produced via modified direct denitration (MDD). PXRD confirmed the bulk identity of NpO 2 , and no additional phases were identified using this method. Analysis of Raman data collected using a 532 nm excitation wavelength indicates that samples are mostly phase pure; however, some variability in spectral features is observed. Analysis of additional spectroscopic data collected with a 785 nm excitation wavelength revealed variability in the relative intensity of spectral features. Raman spectroscopy indicates that the sample is primarily NpO 2 ; however, additional signals indicate possible structural disorder, oxidized species, or potential contributions from other Np phases. To further investigate the possibility of additional phase contributions within the sample of NpO 2 , Raman spectroscopic mapping was employed to examine the homogeneity of the sample produced via DD. From this analysis, we determined that despite variability in the intensity of Raman-active vibrational modes, consistent spectra are obtained throughout the area of the sample investigated. SEM images show aggregates with variable sizes and shapes, with rounded, primary particles possessing an average diameter of approximately 100 nm. Comparison of the results of these multimodal analyses to the literature indicates that the crystal chemical, spectroscopic, and microstructural properties of NpO 2 vary based on synthesis method, even if X-ray diffraction data indicate that the bulk phase is NpO 2 .

Direct denitration↗
DOE OSTI2023

Machine Learning technique for isotopic determination of radioisotopes using HPGe γ-ray spectra

γ-ray spectroscopy is a quantitative, non-destructive technique that may be utilized for the identification and quantitative isotopic estimation of radionuclides. Traditional methods of isotopic determination have various challenges that contribute to statistical and systematic uncertainties in the estimated isotopics. Furthermore, these methods typically require numerous pre-processing steps, and have only been rigorously tested in laboratory settings with limited shielding. Here, in this work, we examine the application of a number of machine learning based regression algorithms as alternatives to conventional approaches for analyzing γ-ray spectroscopy data in the Emergency Response arena. This approach not only eliminates many steps in the analysis procedure, and therefore offers potential to reduce this source of systematic uncertainty, but is also shown to offer comparable performance to conventional approaches in the Emergency Response Application.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Development of a Flow-through Cell for Ultrasonic Extraction (UE)─Single Particle (SP)─ICP-MS─an Approach for Nano/Microparticle Elemental and Isotopic Analysis

Nanotechnology is a salient part of the scientific landscape, and analytical approaches are rapidly evolving to enable small-scale characterization of nano- and microparticle compositions and impurities. Here, a flow-through sonicating cell was developed for direct particle extraction from a silicon wafer and integrated with an inductively coupled plasma–mass spectrometer (ICP-MS) for subsequent elemental and isotopic characterization of the released particles. Ultrasonic extraction (UE)─single particle (SP)─ICP-MS offers controlled particle mobilization from solid substrates and allows for increased sample throughput by eliminating the need for pre-extraction of particles and decreasing sample preparation steps. Coupling this device to an ICP-MS with a time-of-flight (TOF) mass analyzer, it is possible to distinguish unique isotopic compositions of the particles. Both tungsten and nickel isotopically tagged particles, which were deposited on Si wafers, are presented here with analysis via UE─SP─ICP-MS. This approach could support efforts in the fields of particle synthesis, nuclear safeguards and forensics, environmental monitoring, and semiconductor industries in which the detection of particles from substrates and wafers is critical.

Paul, Molly [ORNL] (ORCID:0009000009672055)↗
DOE OSTI2020

Functionalized Polymer Thin Films for Plutonium Capture and Isotopic Screening from Aqueous Sources

The rapid screening of plutonium from aqueous sources remains a critical challenge for nuclear nonproliferation efforts. The determination of trace-level Pu isotopes in water requires offsite sample preparation and analysis; therefore, new methods that combine plutonium purification, concentration, and isotopic screening in a fieldable detection system will provide an invaluable tool for nuclear safeguards. This contribution describes the development and characterization of thin polymer-ligand films for the isolation and concentration of waterborne Pu for direct spectroscopic analyses. Submicron thin films were prepared through spin coating onto Si wafers and consisted of combinations of polystyrene (PS) with dibenzoylmethane, thenoyltrifluoroacetone, and di(2-ethylhexyl)phosphoric acid (HDEHP). Pu uptake studies from solutions at pH from 2.3 to 6.3 indicated that only films containing HDEHP exhibited significant recovery of Pu. High alpha spectroscopy peak energy resolutions were achieved for PS-HDEHP films over a range of film thicknesses from 30 to 250 nm. Furthermore, a separate study was performed to evaluate uptake from a primarily Pu(V) solution where it was observed that doubling the HDEHP loading in the film increased uptake of Pu by an order of magnitude. X-ray photoelectron spectroscopy (XPS) analysis revealed that HDEHP was highly concentrated within the first few nanometers of the film at the higher loading. XPS analysis also revealed that, in the presence of water, HDEHP was stripped from the surface layer of the film at circumneutral pH. While significant losses of ligand were seen in all samples, higher loadings of HDEHP resulted in measurable amounts of ligand retained after a 12-h soak in water. Findings of this study are being used to guide the development of thin-film composite membrane-based detection methods for the rapid, fieldable analysis of Pu in water.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Real-Time Screening for Uranium Enrichment by Paper Spray Ionization Mass Spectrometry for Field Applications

A rapid isotope ratio screening technique for uranium enrichment is demonstrated by utilizing paper spray ionization (PSI) high-resolution mass spectrometry (HRMS). Measurements were conducted using an ambient ionization mass spectrometer coupled to a custom-made JEOL PSI attachment apparatus, with de minimus sample preparation requirements. The current method detection limit for individual isotopes (e.g., 235 U and 238 U) is approximately 50 pg, with subsequent optimization expected to further improve U isotopic sensitivity. The PSI analytical method described herein can support rapid analysis (both in-field and in-lab screening) of isotopes-of-interest, as demonstrated by empirical differentiation of depleted uranium (DU) and low enriched uranium (LEU) analytical aliquots. Furthermore, this analytical workflow holds promise for applications in nuclear forensics, international nuclear safeguards, and nonproliferation missions.

Anions↗