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Mace, Emily K.

Publications and source records attributed to Mace, Emily K..

Reduction of detection limit and quantification uncertainty due to interferent by neural classification with abstention

Many measurements in the physical sciences can be cast as counting experiments, where the number of occurrences of a physical phenomenon informs the prevalence of the phenomenon's source. Often, detection of the physical phenomenon (termed signal) is difficult to distinguish from naturally occurring phenomena (termed background). In this case, the discrimination of signal events from background can be performed using classifiers, and they may range from simple, threshold-based classifiers to sophisticated neural networks. These classifiers are often trained and validated to obtain optimal accuracy, however we show that the optimal accuracy classifier does not generally coincide with a classifier that provides the lowest detection limit, nor the lowest quantification uncertainty. Here, we present a derivation of the detection limit and quantification uncertainty in the classifier-based counting experiment case. We also present a novel abstention mechanism to minimize the detection limit or quantification uncertainty a posteriori. We illustrate the method on two data sets from the physical sciences, discriminating Ar-37 and Ar-39 radioactive decay from non-radioactive events in a gas proportional counter, and discriminating neutrons from gammas in an inorganic scintillator and report results therefrom.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Measurements of Argon-39 from locations near historic underground nuclear explosions

Measurement of radioactive gas seepage from an underground nuclear explosion is one of the primary methods to confirm whether an event was nuclear in nature. Radioactive noble gas indicators that are commonly targeted by such measurements (e.g. 133Xe, 37Ar) have half-lives of 35 days or less. Argon-39, an activation product similar to 37Ar, is produced by the interaction between neutrons and potassium in the surrounding geology and has a half-life of 269 years. Measurements taken at three sites near three historic underground nuclear test locations at the Nevada National Security Site have all shown highly elevated levels of 39Ar in subsurface air decades after the test events. Elevated levels of 39Ar (30-50 times background) were also detected in atmospheric air collected roughly 30 cm above ground level near two of these sites, and outside the entrance of the one tunnel site. These measurements demonstrate that 39Ar has the potential to be a long-term signature of an underground nuclear event which can be reliably detected at the surface or in the shallow subsurface. This radionuclide detection of an underground nuclear event decades after the event takes place is in contrast to the commonly held assumption that detecting underground nuclear events via radionuclides at the surface needs to be done in a matter of months. Depending upon what further studies show about the robustness of this signature in a variety of geological settings, it may in fact be easy to detect underground nuclear events at the surface for a very long time post-detonation.

Johnson, Christine M.↗

Measurements of the emanation of 37Ar and 39Ar from irradiated rocks and powders

The emanation fraction of radionuclides has been highlighted as a known source of uncertainty in the estimation of radionuclide source signatures from underground nuclear tests and other nuclear activities, particularly in the case of activation products. A system was developed at Pacific Northwest National Laboratory to quantify the emanation fraction of argon from samples ranging in particle size from powder to small rocks. Seven materials, two powders and five rock types, were neutron irradiated and the emanation fraction of 37Ar was measured. Additional measurements were made of the 39Ar emanation for four of these materials.

Johnson, Christine M.↗

Comparison of near-background concentrations of Argon-37 and Xenon-133 in the Atmosphere

Radioisotopes of noble gases xenon and argon can be important indicators of underground nuclear explosions. The Comprehensive Nuclear-Test-Ban Treaty (CTBT) includes monitoring capabilities to identify potential nuclear explosions conducted in violation of the CTBT. This monitoring currently focuses on measurement of the xenon isotopes 133Xe, 135Xe, 131mXe and 133mXe. However, it is predicted that within 100 days of an underground nuclear explosion (UNE) 37Ar would be released to the atmosphere at higher concentrations than xenon isotopes (Haas et al. 2010) and with a higher signal to background ratio, depending on the radioxenon background levels. Therefore, inclusion of 37Ar measurement capabilities at atmospheric International Monitoring System (IMS) stations may represent an improvement in the capability to detect a nuclear explosion. At an IMS station, it could be difficult to determine what constitutes an elevated concentration as a result of an UNE without first understanding the expected range of background concentrations. This work describes our analysis of atmospheric samples for 37Ar to evaluate the range of background concentrations. Samples were collected at multiple locations, with approximately half coming from a sampler co-located with an IMS xenon monitoring station (RN75). The range of 37Ar concentrations measured in atmospheric air samples was relatively narrow; for samples considered detectable, the minimum and maximum measured concentrations were 0.56 and 2.3 mBq/m3, respectively. Comparison of 37Ar and 133Xe concentrations measured at the IMS station indicated some correlation between the measured concentrations. The results presented here demonstrate the capability to detect background concentrations of 37Ar in atmospheric air and provide a basis for potential implementation of 37Ar monitoring at IMS stations.

Fritz, Brad G.↗

Background Concentrations of Argon-39 in Shallow Soil Gas

While radioisotopes of noble gases are known to be indicators of underground nuclear explosions (UNE), McIntyre et al. (2017) was the first to report the presence of 39Ar in shallow soil gas in association with a decades old UNE. While this finding hinted at the potential application of 39Ar to be used as an indicator of an UNE, doing so would also require an understanding of the natural concentrations of 39Ar present in soil gas. Without knowing the expected range and variability of naturally occurring concentrations of 39Ar, it is difficult to determine what measured concentrations would be indicative of an elevated concentration. This paper presents results from 16 soil gas samples and three atmospheric air samples collected from various locations across the western United States. Shallow soil gas samples were collected into self-contained underwater breathing apparatus (SCUBA) tanks using a custom-built soil gas sampling system and then processed and analyzed for 39Ar. The measured concentrations of 39Ar varied from atmospheric air concentrations to about 3.5 times atmospheric air concentrations. The variation in concentration was primarily attributed to the latitude the sample was collected at, which was consistent with previous work (Johnson et al. 2015). The results presented here represent the first measurements of natural background 39Ar concentrations in shallow soil gas. This data will be necessary if 39Ar is to be used as an indicator of UNE.

Fritz, Brad G.↗

Configuration and impurity quantification of AmLi sources using radiography and gamma spectroscopy

This paper presents the non-destructive assay of two AmLi sources used for detector characterization and active interrogation at PNNL, identified as MRC-101 and MRC-103. First, a detailed description of the internal configuration of 2724-BT encapsulated MRC sources is established. X-ray radiographs of the AmLi sources are reported for the first time to verify the dimensions and orientation of the encapsulation. Notably, a density variation was observed as a contrast change across the height of the source cavities. Contrary to commonly made assumptions in literature, it is indirectly observed that the AmLi source/target material only occupies a portion of the source cavity. The intensity of the prompt gamma-rays resulting from the inelastic scatter of alpha particles on 7Li was used to calculate the mass ratios of LiH:AmO2. The gamma-ray spectra revealed the presence of numerous impurities in both source and target material (243Am, 237Np, 154Eu, 23Na, and 9Be). Neutron-gamma production ratios were applied to the intensity of the Doppler-broadened peaks from alpha-induced reactions with 7Li, 9Be, and 23Na to calculate neutron rates for both sources. A neutron/alpha production yield (derived in this work) was then related to the atomic concentration of these isotopes to find the approximate masses within each source. Ultimately, the AmLi source density was estimated with prompt gamma analysis based on partial source volumes as 0.45±0.08 g/cm^3.

DTRA, AmLi, neutron↗

Characterization of Two Extraordinary AmLi Neutron Sources

Two legacy AmLi sources, MRC-101 and MRC-103, are routinely used for neutron detector characterization and testing campaigns that Pacific Northwest National Laboratory manages for the Defense Threat Reduction Agency within the U.S. Department of Defense. However, applicability of source measurement data has been substantially limited due to the lack of original manufacturer documentation and cross comparison to other sources. This paper summarizes results of the measurement campaign conducted to better quantify source radionuclide content, neutron energy spectrum and emission rate of the AmLi sources. The source characterization study consisted of three major consecutive measurement exercises. First, gamma spectrometry measurements using a high purity germanium detector were used to estimate the radionuclide content and potential impurities of the AmLi sources. Then neutron spectral measurements were taken to determine the unique neutron energy distribution. Finally, assessments of the total neutron yields of the sources were made with measurements in a neutron well counter. The neutron detection efficiency for these measurements was determined via detailed Monte Carlo modeling based on the neutron energy distribution measured with the rotating neutron spectrometer. The most exciting and unexpected finding of the study was a significant contamination of the source material with beryllium, contributing up to 17% to the total neutron emission rate and correspondingly changing the neutron energy spectrum. Also, the obtained lithium-only portion of the measured energy distribution of the sources was compared against several AmLi spectra previously reported by different researchers.

AWCC, AmLi, beryllium contamination, neutron spect↗

UNESE Argon-39 Measurement Techniques: Developing an above-ground Argon-39 Measurement Capability

The Underground Nuclear Explosion Signatures Experiment (UNESE) sought to use 37 Ar as a tracer for measuring noble-gas migration in the soil surrounding historic Underground Nuclear Explosions (UNE). One unexpected observation was the presence of the much longer-lived isotope 39 Ar from historic UNEs. Quantifying the activity of 39 Ar proved difficult due to the lack of capability to measure significantly-above-background levels of 39 Ar and a general discomfort to repeatedly expose Ultra-Low-Background Proportional Counters (ULBPCs) to significant radioactivity. Because the whole-air samples collected for the 37 Ar tracer measurement were already being measured on the above-ground argon capability, it was decided to expand that capability to include 39 Ar. This document describes the efforts required to achieve quantitative reporting of the 39 Ar backgrounds measured during experiments at the sites of the historic Barnwell and Disko Elm UNEs.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurements of emanation of Ar-37 and Ar-39 from irradiated rocks and powders

The emanation fraction of radionuclides has been highlighted as a known source of uncertainty in the estimation of radionuclide source signatures from underground nuclear tests and other nuclear activities, particularly in the case of activation products. A system was developed at Pacific Northwest National Laboratory to quantify the emanation fraction of argon from samples ranging in particle size from powder to small rocks. Seven materials, two powders and five rock types, were irradiated with fission spectrum neutrons and the emanation fraction of 37 Ar was measured. Additional measurements were made of the 39 Ar emanation for four of these materials.

36 MATERIALS SCIENCE↗

Analysis methods for quantifying Xe-127 samples from the UNESE project

In the Underground Nuclear Explosions Signatures Experiment (UNESE) radioactive 37 Ar and 127 Xe were used as tracers in subsurface migration experiments. As part of the experiment, methods were developed to quantify 127 Xe via β-γ coincidence spectroscopy. Later examination of the results highlighted a weakness of this analysis method in samples with no 127 Xe present, so a reanalysis of samples was performed to identify those which were falsely identified as having 127 Xe present. Ongoing work to develop a new analysis method with targeted regions of interest is also described. Measurements were also performed to quantify the concentration of 127 Xe and 37 Ar which were injected as part of UNESE Phase 2. A best value for the concentration of 37 Ar and 127 Xe was determined and reported here for use in future analyses of the UNESE Phase 2 results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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↗

Measurement of Argon-37 Background Concentrations in the Atmosphere

Radioisotopes of noble gases, primarily xenon and argon, are important indicators of underground nuclear explosions. The Comprehensive Nuclear-Test-Ban Treaty (CTBT) includes monitoring capabilities to identify potential nuclear explosions conducted in violation of the CTBT. This monitoring currently focuses on measurement of the xenon isotopes 133 Xe, 135 Xe, 131 mXe and 133 mXe. However, it is predicted that within 100 days of an underground nuclear explosion (UNE) 37 Ar would be released to the atmosphere at higher concentrations than xenon isotopes (Haas et al. 2010). Therefore, inclusion of 37 Ar measurement capabilities at atmospheric International Monitoring System (IMS) stations could improve the capability to detect a nuclear explosion. At an IMS station, it could be difficult to determine what constitutes an elevated concentration as a result of an UNE without first understanding the expected range of background concentrations. This work describes our analysis of atmospheric samples for 37 Ar to evaluate the range of background concentrations. The range of 37 Ar concentrations measured in atmospheric air samples was relatively narrow ranging between less than 1 mBq/m 3 to greater than 2 mBq/m 3 . The average atmospheric concentration of all samples was 0.98 mBq/m 3 , with a standard deviation of 0.5 mBq/m 3 . This is consistent with previous published results. The results presented here demonstrate the capability to detect background concentrations of 37 Ar in atmospheric air.

61 RADIATION PROTECTION AND DOSIMETRY↗