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At least 37 records · Page 2

NMIS/FNMIS Comparison for US DOE Office of Nuclear Verification

A comparison of the characteristics of the Nuclear Materials Identification System (NMIS) and its more fieldable version that was developed for future treaty applications, the Fieldable Nuclear Materials Identification System (FNMIS), is presented. Both systems were developed for the US Department of Energy (DOE) Office of Nuclear Verification (ONV). Under the Warhead Safety and Security Exchange Agreement, NMIS was also jointly developed with the Russian Federation. The configuration of the systems and their characteristics are described. In addition, the capabilities, advantages and disadvantages, and a comparison fast-neutron transmission imaging measurement is presented. The comparison measurements gave essentially the same results because the software and imaging apparatus have the same capabilities, with the FNMIS completing the measurements slightly faster. NMIS is an open system that is more easily modified for research applications and is not suitable for the ONV mission, and FNMIS is compatible with an information barrier, which is more useful for ONV applications.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Portable Waveguide-Based Optical Biosensor

Rapid, on-site diagnostics allow for timely intervention and response for warfighter support, environmental monitoring, and global health needs. Portable optical biosensors are being widely pursued as a means of achieving fieldable biosensing due to the potential speed and accuracy of optical detection. We recently developed the portable engineered analytic sensor with automated sampling (PEGASUS) with the goal of developing a fieldable, generalizable biosensing platform. Here, we detail the development of PEGASUS’s sensing hardware and use a test-bed system of identical sensing hardware and software to demonstrate detection of a fluorescent conjugate at 1 nM through biotin-streptavidin chemistry.

47 OTHER INSTRUMENTATION↗

High Throughput Argon-37 Field System

We report Pacific Northwest National Laboratory (PNNL) has developed a unique fieldable 37 Ar measurement system designed to measure 37 Ar activity concentrations from soil gas samples to detect above ground and underground nuclear explosions. The Argon-37 Field System is modular in design to accommodate both chemical processing and nuclear detection. The system can be packed into shipping crates and shipped to a location near where the sampling is taking place. The system can process six 2-m 3 whole-air samples in 24 hours and can measure the 37 Ar activity in each of the samples using six proportional counters. The proportional counters, designed and built at PNNL, are surrounded with both active and passive shielding to reduce background and can achieve a minimum detection concentration of 10 mBq/m 3 of 37 Ar in whole-air equivalent. The Argon-37 Field System has undergone extensive testing against rigorous requirements to assure the system meets the needs of the noble gas nuclear explosion monitoring community.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Preliminary Figures of Merit for Isotope Ratio Measurements: The Liquid Sampling-Atmospheric Pressure Glow Discharge Microplasma Ionization Source Coupled to an Orbitrap Mass Analyzer

ABSTRACT In order to meet a growing need for fieldable mass spectrometer systems for precise elemental and isotopic analyses, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) has a number of very promising characteristics. One key set of attributes that await validation deals with the performance characteristics relative to isotope ratio precision and accuracy. Due to its availability and prior experience with this research team, the initial evaluation of isotope ratio (IR) performance was performed on a Thermo Scientific Exactive Orbitrap instrument. While the mass accuracy and resolution performance for orbitrap analyzers are very well documented, no detailed evaluations of the IR performance have been published. Efforts described here involve two variables: the inherent IR precision and accuracy delivered by the LSAPGD microplasma and the inherent IR measurement qualities of orbitrap analyzers. Important to the IR performance, the various operating parameters of the orbitrap sampling interface, HCD dissociation stage, and ion injection/data acquisition have been evaluated. The IR performance for a range of other elements, including natural, depleted, and enriched uranium isotopes was determined. In all cases the precision and accuracy are degraded when measuring low abundance (<0.1% isotope fractions). In the best case, IR precision on the order of 0.1 %RSD can be achieved, with values of 1-3 %RSD observed for low-abundance species. The results suggest that the LSAPGD is a very good candidate for field deployable MS analysis and that the high resolving powers of the orbitrap may be complemented with a here-to-fore unknown capacity to deliver high-precision isotope ratios.

Environmental Molecular Sciences Laboratory↗

Pressure-Sensitive Adhesive Combined with Paper Spray Mass Spectrometry for Low-Cost Collection and Analysis of Drug Residues

Illicit drug use causes over half a million deaths worldwide every year. Drugs of abuse are commonly smuggled through customs and border checkpoints and, increasingly, through parcel delivery services. Improved methods for detection of trace drug residues from surfaces are needed. Such methods should be robust, fieldable, sensitive, and capable of detecting a wide range of drugs. In this work, commercially produced paper with a pressure-sensitive adhesive coating was utilized for the collection and analysis of trace drug residues by paper spray mass spectrometry (MS). This modified substrate was used to combine sample collection of drug residues from surfaces with rapid detection using a single paper spray ticket. The all-in-one ticket was used to probe different surfaces commonly encountered in forensic work including clothing, cardboard, glass, concrete, asphalt, and aluminum. A total of 10 drugs (acetyl fentanyl, fentanyl, clonazolam, cocaine, heroin, ketamine, methamphetamine, methylone, U-47700, and XLR-11) were evaluated and found to be detectable in the picogram range using a benchtop mass spectrometer and in the low nanogram range using a portable ion trap MS. Finally, the novel approach demonstrates a simple yet effective sampling strategy, allowing for rapid identification from difficult surfaces via paper spray mass spectrometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Rapid Quantification of 237 U Specific Activity for Nuclear Forensics

In the event of an unattributed nuclear explosion, rapid assessment of the short-lived uranium isotope activity and mass can provide valuable information for subsequent forensic analysis. Rapid analysis in the field is enabled by using microfluidic chemistry and deployable instrumentation. Here, this work presents a flow chemistry system, controlled in LabVIEW, that integrates three functionalities: (1) selective extraction of uranium from the sample matrix via a 3D-printed supported liquid membrane module; (2) UV–visible absorbance spectrophotometry to measure the total uranium concentration in the strip flow; and (3) a portable CdTe γ-ray spectrometer coupled to a 3D-printed flow cell to measure 237 U activity concentration in the strip solution. The system was calibrated using standard solutions, and its functionality was demonstrated using a solution of depleted uranium spiked with 237 U. Uranium concentrations of 40–5000 μg/mL were directly quantified online using a 100 mm optical flow cell, while concentrations of 0.5–10 μg/mL were quantified online using a colorimetric reagent. The mass concentration measurement takes approximately 60 min while the activity concentration via γ-ray spectrometry varies depending on the activity of 237 U, with 1 kBq/mL requiring about 30 min of acquisition time to obtain <10% uncertainty at 1σ. This platform provides a fieldable approach for quantifying uranium mass and radioactivity relevant to postdetonation nuclear debris.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermochemical Properties of a Water-Soluble Zr(IV)-Flavonolate Complex for Fluoride Sensing

Detection of fluoride in water samples is critical for monitoring many chemical, environmental, and biological processes, however, these measurements often rely on costly instrumentation. Here, this situation has motivated the design of simple to use, fieldable fluoride sensors. Previously, a fluorometric sensor based on (EDTA)­Zr­(H 2 O) 2 (EDTA = ethylenediamine-N,N,N′,N′-tetraacetate) and 3-hydroxyflavone (FlvH) was reported for fluoride detection in ethanol-H 2 O mixtures. Herein, we report the synthesis and characterization of the previously proposed Zr­(IV)-flavonolate complex as the dimethylammonium salt, [(EDTA)­Zr­(Flv)]­[NMe 2 H 2 ] (Flv = 3-hydroxyflavonolate), and detail its utility for aqueous fluoride sensing. This species exhibits an intense blue fluorescence upon excitation with near-UV light (λ ex = 390 nm; λ em = 460 nm) that is quenched in the presence of NaF (100 mM acetate buffer, pH = 5) with good sensitivity (LOD = 20.9 nM; [F – ] from 10 –8 to 10 –4 M) under neat aqueous conditions. The equilibrium constant (K eq = 1.26 ± 0.00184 × 10 8 M –2 ) and free energy (Δ$G^°_{\textrm{rxn}}$ = –11.0 kcal mol –1 ) were determined under the conditions used for fluoride sensing, indicating a highly favorable reaction with F – in water. Finally, we developed paper-based sensing strips for qualitative fluoride sensing by immobilizing the sensor in a deposited gel enabling good selectivity and reduced interference due to slower ion diffusion.

aqueous chemistry↗

Design, construction, and validation of an in-situ groundwater trace element analyzer with applications in carbon storage

Abstract It is estimated that carbon emissions should reach net-zero by 2050 to meet important climate targets. Carbon capture is likely necessary to reach these targets, requiring a long-term storage solution such as geological carbon sequestration. However, as with any subsurface activity, leakage can occur, potentially impacting groundwater quality near the storage site. Rapid detection is essential to mitigate damage to this resource. Since CO 2 will acidify groundwater, the concentrations of acid soluble minerals and associated cations will increase. Thus, an in-situ, real-time element analysis system based on laser-induced breakdown spectroscopy (LIBS) is under development to monitor these elements. The system splits the traditional LIBS system into a miniature, all-optical sensor head built around a passively Q-switch laser fiber coupled to a control unit. Previous work has validated the LIBS technique for use at high pressure as well as the split system design. In this work, a fieldable prototype sensor is developed and tested in an onsite monitoring well where trace elements concentrations (approx. 0–3 ppm) were tracked over 20 days. These concentrations varied in response to local rainfall, diluting with increased rain, demonstrating the ability of a LIBS-based sensor to track trace elements under real-world conditions.

54 ENVIRONMENTAL SCIENCES↗

Fully Additively Manufactured Wetted Foam Capsules for Inertial Confinement Fusion

In the pursuit of realizing reliable clean energy generation via inertial confinement fusion (ICF), wetted foam (WF) capsule targets have long been coveted due to their potential to simplify the target fielding process and suppress hydrodynamic instabilities and material mixing that limit achievable energy output, yet producing and deploying a WF target has proven challenging. Here, in this work, we demonstrate the design, fabrication, metrology, and testing of fully additively manufactured (AM) foam-lined capsules using two-photon polymerization (2PP) for ICF. We successfully fielded an AM polymeric foam capsule with a 3-mm outer diameter, a nominally 15-µm-thick solid outer layer, a 120-µm-thick inner foam layer, and a 250-µm outer diameter copper fill tube on the National Ignition Facility for a polar direct-drive shot, and we showcase deuterium wetting of the capsule foam layer inside an ignition target proofing station. Our exploration showed that 2PP can produce fieldable targets with complex geometries and potentially shorten the design iteration turnaround time and the overall target fabrication time.

Target↗

A Spherical Active Coded Aperture for 4π Gamma-ray Imaging

Gamma-ray imaging facilitates the efficient detection, characterization, and localization of compact radioactive sources in cluttered environments. Fieldable detector systems employing active planar coded apertures have demonstrated broad energy sensitivity via both coded aperture and Compton imaging modalities. But, planar configurations suffer from a limited field-of-view, especially in the coded aperture mode. In order to improve upon this limitation, we introduce a novel design by rearranging the detectors into an active coded spherical configuration, resulting in a 4pi isotropic field-of-view for both coded aperture and Compton imaging. This work focuses on the low- energy coded aperture modality and the optimization techniques used to determine the optimal number and configuration of 1 cm 3 CdZnTe coplanar grid detectors on a 14 cm diameter sphere with 192 available detector locations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Vintage electronics for trusted radiation measurements and verified dismantlement of nuclear weapons

Information barriers are trusted measurement systems to confirm the authenticity of nuclear warheads based on their radiation signatures. Traditional inspection systems rely on complex electronics both for data acquisition and processing. Several research efforts have produced prototype systems, but it has proven difficult to demonstrate that hidden switches and side channels do not exist. After almost thirty years of research and development, no viable and widely accepted system has emerged. We pursue a fundamentally different approach: Our prototype of an inspection system uses vintage hardware built around a 6502 processor. The processor uses 8-micron technology and has only about 4,200 transistors. Vintage electronics may have a number of important advantages for applications where two parties need to simultaneously establish trust in the hardware used. CPUs designed in the distant past, at a time when their use for sensitive measurements was never envisioned, drastically reduce concerns that the other party implemented backdoors or hidden switches on the hardware level. We demonstrate the performance of a prototype system using an Apple IIe and a custom-made open-source data-processing board connected to a standard sodiumiodide radiation detector for low-resolution gamma spectroscopy. Data processing and analysis is exclusively done on the Apple IIe hardware. We show that subtle differences in radiation signatures can be detected in 2–3 minutes based on the result of a simple chi-squared test. Vintage electronics may therefore offer a new path toward fieldable, trusted information barriers.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Atomic Beam Laser Spectrometer for In-field Isotopic Analysis

This is a powerpoint presentation for the DTRA quarterly program review that goes into detail about the atomic beam laser spectrometer for in-field isotopic analysis. The project goals are the following: analysis of post-detonation debris, determination of U and Pu isotopic composition, and fieldable prototype: < 2ft 3 , < 1000W.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Possible Nuclear Safeguards Applications: Workshop on Next-Generation Laser Compton Gamma Source

These are a set of slides for the development of a next-generation photon source white paper. The following topics are covered in these slides: Nuclear Safeguards; The Nuclear Fuel Cycle; Precise isotopic determination via NRF; UF 6 Enrichment Assay; and Non-Destructive Assay of Spent Nuclear Fuel. In summary: A way to non-destructively measure precise isotopics of ~kg and larger samples has multiple uses in nuclear safeguards; Ideally this is a compact, fieldable device that can be used by international inspectors. Must be rugged and reliable; A next-generation source can be used as a testing ground for these techniques as technology develops.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Analyses of Field Test Data at the Atucha-1 Spent Fuel Pools

A field test was conducted at the Atucha-1 spent nuclear fuel pools to validate a software package for gross defect detection that is used in conjunction with the inspection tool, Spent Fuel Neutron Counter (SFNC). A set of measurements was taken with the SFNC and the software predictions were compared with these data and analyzed. The data spanned a wide range of cooling times and a set of burnup levels leading to count rates from the several hundreds to around twenty per second. The current calibration in the software using linear fitting required the use of multiple calibration factors to cover the entire range of count rates recorded. The solution to this was to use power regression data fitting to normalize the predicted response and derive one calibration factor that can be applied to the entire set of data. The resulting comparisons between the predicted and measured responses were generally good and provided a quantitative method of detecting missing fuel in virtually all situations. Since the current version of the software uses the linear calibration method, it would need to be updated with the new power regression method to make it more user-friendly for real time verification and fieldable for the range of responses that will be encountered.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Scoping study to expedite development of a field deployable and portable instrument for UF6 enrichment assay

The primary objective of the present study is to identity the most promising, viable technologies that are likely to culminate in an expedited development of the next-generation, field-deployable instrument for providing rapid, accurate, and precise enrichment assay of uranium hexafluoride (UF6). UF6 is typically involved, and is arguably the most important uranium compound, in uranium enrichment processes. As the first line of defense against proliferation, accurate analytical techniques to determine the uranium isotopic distribution in UF6 are critical for materials verification, accounting, and safeguards at enrichment plants. As nuclear fuel cycle technology becomes more prevalent around the world, international nuclear safeguards and interest in UF6 enrichment assay has been growing. At present, laboratory-based mass spectrometry (MS), which offers the highest attainable analytical accuracy and precision, is the technique of choice for the analysis of stable and long-lived isotopes. Currently, the International Atomic Energy Agency (IAEA) monitors the production of enriched UF6 at declared facilities by collecting a small amount (between 1 to 10 g) of gaseous UF6 into a sample bottle, which is then shipped under chain of custody to a central laboratory (IAEA’s Nuclear Materials Analysis Laboratory) for high-precision isotopic assay by MS. The logistics are cumbersome and new shipping regulations are making it more difficult to transport UF6. Furthermore, the analysis is costly, and results are not available for some time after sample collection. Hence, the IAEA is challenged to develop effective safeguards approaches at enrichment plants. In-field isotopic analysis of UF6 has the potential to substantially reduce the time, logistics and expense of sample handling. However, current laboratory-based MS techniques require too much infrastructure and operator expertise for field deployment and operation. As outlined in the IAEA Department of Safeguards Long-Term R&D Plan, 2012–2023, one of the IAEA long-term R&D needs is to “develop tools and techniques to enable timely, potentially real-time, detection of HEU (Highly Enriched Uranium) production in LEU (Lowly Enriched Uranium) enrichment facilities” (Milestone 5.2). Because it is common that the next generation of analytical instruments is driven by technologies that are either currently available or just now emerging, one reasonable and practical approach to project the next generation of chemical instrumentation is to track the recent trends and to extrapolate them. This study adopted a similar approach, and an extensive literature review on existing and emerging technologies for UF6 enrichment assay was performed. The competitive advantages and current limitations of different analytical techniques for in-field UF6 enrichment assay were then compared, and the main gaps between needs and capabilities for their field use were examined. Subsequently, based on these results, technologies for the next-generation field-deployable instrument for UF6 enrichment assay were recommended. The study was organized in a way that a suite of assessment metric was first identified. Criteria used in this evaluation are presented in Section 1 of this report, and the most important ones are described briefly in the next few paragraphs. Because one driving force for in-field UF6 enrichment assay is related to the demanding transportation regulation for gaseous UF6, Section 2 contains a review of solid sorbents that convert and immobilized gaseous UF6 to a solid state, which is regarded as more transportation friendly and is less regulated. Furthermore, candidate solid sorbents, which show promise in mating with existing and emerging assay technologies, also factor into technology recommendations. Extensive literature reviews on existing and emerging technologies for UF6 enrichment assay, covering their scientific principles, instrument options, and current limitations are detailed in Sections 3 and 4, respectively. In Section 5, the technological gaps as well as start-of-the-art and commercial off-the-shelf components that can be adopted to expedite the development of a fieldable or portable UF6 enrichment-assay instrument are identified and discussed. Finally, based on the results of the review, requirements and recommendations for developing the next-generation field-deployable instrument for UF6 enrichment assay are presented in Section 6.

36 MATERIALS SCIENCE↗

R200 Spectrometer with Frisch-grid Cadmium Zinc Telluride (CZT)

The goal of this project is to demonstrate an engineering prototype of a gamma ray spectrometer that uses Cadmium Zinc Telluride (CZT) in a configuration comprised of an array of position-sensitive virtual Frisch grid (PSVFG) detectors and show its capability to perform functions that would be useful to the IAEA. The detectors should achieve energy resolution of 2-3% at 200 keV and <1% at > 662 keV (at temperature <30°C), thereby outperforming all hand-held instruments currently in use other than cryogenically cooled germanium. BNL is working to transfer the technology to an industrial partner so that robust, fieldable instruments can be manufactured.

36 MATERIALS SCIENCE↗

Magnetic Detection of Chemical Threats

Los Alamos researchers have developed a technology to quickly detect chemical threats using a fieldable detector that provides real-time detection to ensure safety for warfighters, agricultural workers, and the general public. Traditional laboratory-based detection does not allow for agile response to threats on the battlefield or to our food supply chain. Our portable detector brings the laboratory to the field for real-time detection of chemical agents in samples without needing to send the samples to a remote location for analysis. This technology fits a market need in public safety, military sensor design, and pesticide detection. We have proven that this technology works on the benchtop, and are working to miniaturize the system to enable deployment. We are seeking qualified licensing or CRADA partners to finalize development of this system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Predicting Ionizing Radiation Exposure (LDRD Final Report)

Rapid, low-cost, easy-to-use devices are needed for screening large populations potentially exposed to ionizing radiation following accidental or intentional release of radioactive materials. Measurements of radiation responsive messenger RNA (mRNA) biomarkers using fieldable devices could provide such a tool. mRNA expression level changes may be useful for discriminating between exposed individuals and the worried well and estimating the radiation dose received even days after exposure. Loop mediated isothermal amplification, or LAMP, is an established nucleic acid amplification technique that provides key advantages for use in low cost, portable instruments. We proposed to use LAMP to determine if the expression level of one or a small number of radiation responsive biomarkers can be used to discriminate unexposed cells from ionizing radiation (IR)-exposed cells. If successful, this methodology could potentially be transitioned to portable detection technology for use in population screening after large-scale events. Our approach involved designing quantitative, real-time, reverse transcriptase loop-mediated isothermal amplification (RTLAMP) assays for a panel of published IR-responsive mRNA biomarkers and control genes. This assay panel was then tested on mRNA isolated from white blood cells, lymphocyte cell lines and samples from internally dosed individuals. We used standard curves to quantify mRNA copy number along with the comparative Ct method to measure relative mRNA expression changes. We were able to generate quantitative and comparative gene expression changes for many of the samples evaluated. Although promising in its potential to measure gene expression, the technique suffered when attempting to amplify target genes with very low background RNA expression levels, in particular, FDXR in controls samples. Future work should focus on optimizing the RT-LAMP reaction for low RNA expression level targets allowing for the generation of validated assay panels.

59 BASIC BIOLOGICAL SCIENCES↗