Absolute gas counting (AGC) was applied to two gas blends of 85Kr in argon-methane (P10) counting gas to establish a high-precision specific activity (Bq/cm3) reference value for characterizing 85Kr detection efficiency for groundwater age dating measurements. The AGC or length-compensated technique has been utilized by the metrology community for decades and is an accepted method for developing radioactive gas standards. The AGC capability at Pacific Northwest National Laboratory (PNNL) uses a set of nine unequal-length proportional counters with precisely-measured internal volumes, and a gas loading system with high-precision pressure and temperature sensors.A series of AGC measurements were collected at multiple pressures to determine the inverse pressure relationship (1/P) for 85Kr and define a wall-effect correction that accounts for events decaying into the detector wall and not depositing sufficient energy in the gas to be detected. In addition to the wall-effect, two additional corrections were evaluated and are discussed in detail. Specifically, the threshold effect which accounts for events deposited below the analysis threshold and a detection efficiency as a function of detector volume effect that was observed during analysis. A robust uncertainty model was developed using the Guide to the expression of Uncertainty in Measurements (GUM) approach. The combination of carefully scrutinized correction factors, precise measurements of pressure, temperature and detector volume, and robust counting statistics resulted in the determination of high-precision specific activity values with 0.50% or less total combined uncertainty for two Kr-in-P10 reference gas standards (KP10) that will enable new groundwater age-dating measurements at PNNL.

With the continuing development of fusion energy, it is reasonable to be concerned about contamination from the potential release of tritiated water (HTO) plumes, as well as the oxidation of atmospheric tritiated hydrogen gas (HT) releases in nearby soils. We build on past studies by examining oxidation rates of HT to HTO at two sites representing dry and moist soil. We also examine diurnal changes to better constrain rates of microbial HT oxidation and subsequent deposition into soils. We estimate the potential effects of an HTO plume resulting from an oxidation HT. This methodology framework is expected to be useful in the determination of potential health and environmental impacts from HTO as a result of HT releases.

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. 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 photons in an inorganic scintillator and report results therefrom.

Groundwater is an important source of drinking and irrigation water. Dating groundwater informs its vulnerability to contamination and aids in calibrating flow models. Here, we report measurements of multiple age tracers (14C, 3H, 39Ar, and 85Kr) and parameters relevant to dissolved inorganic carbon (DIC) from 17 wells in California's San Joaquin Valley (SJV), an agricultural region that is heavily reliant on groundwater. We find evidence for a major mid-20th century shift in groundwater DIC input from mostly closed- to mostly open-system carbonate dissolution, which we suggest is driven by input of anthropogenic carbonate soil amendments. Crucially, enhanced open-system dissolution, in which DIC equilibrates with soil CO2, fundamentally affects the initial 14C activity of recently recharged groundwater. Conventional 14C dating of deeper SJV groundwater, assuming an open system, substantially overestimates residence time and thereby underestimates susceptibility to modern contamination. Because carbonate soil amendments are ubiquitous, other groundwater-reliant agricultural regions may be similarly affected.

Proportional electroluminescence (EL) in noble gases is used in two-phase detectors for dark matter searches to record (in the gas phase) the ionization signal induced by particle scattering in the liquid phase. The “standard” EL mechanism is considered to be due to noble gas excimer emission in the vacuum ultraviolet (VUV). In addition, there are two alternative mechanisms, producing light in the visible and near infrared (NIR) ranges. The first is due to bremsstrahlung of electrons scattered on neutral atoms (“neutral bremsstrahlung”, NBrS). The second, responsible for electron avalanche scintillation in the NIR at higher electric fields, is due to transitions between excited atomic states. In this work, we have for the first time demonstrated two alternative techniques of the optical readout of two-phase argon detectors, in the visible and NIR range, using a silicon photomultiplier matrix and electroluminescence due to either neutral bremsstrahlung or avalanche scintillation. The amplitude yield and position resolution were measured for these readout techniques, which allowed to assess the detection threshold for electron and nuclear recoils in two-phase argon detectors for dark matter searches. To the best of our knowledge, this is the first practical application of the NBrS effect in detection science.

Large liquid argon detectors offer one of the best avenues for the detection of galactic weakly interacting massive particles (WIMPs) via their scattering on atomic nuclei. The liquid argon target allows exquisite discrimination between nuclear and electron recoil signals via pulse-shape discrimination of the scintillation signals. Atmospheric argon (AAr), however, has a naturally occurring radioactive isotope, ^39Ar, a β emitter of cosmogenic origin. For large detectors, the atmospheric ^39Ar activity poses pile-up concerns. The use of argon extracted from underground wells, deprived of ^39Ar, is key to the physics potential of these experiments. The DarkSide-20k dark matter search experiment will operate a dual-phase time projection chamber with 50 tonnes of radio-pure underground argon (UAr), that was shown to be depleted of ^39Ar with respect to AAr by a factor larger than 1400. Assessing the ^39Ar content of the UAr during extraction is crucial for the success of DarkSide-20k, as well as for future experiments of the Global Argon Dark Matter Collaboration (GADMC). This will be carried out by the DArT in ArDM experiment, a small chamber made with extremely radio-pure materials that will be placed at the centre of the ArDM detector, in the Canfranc Underground Laboratory (LSC) in Spain. The ArDM LAr volume acts as an active veto for background radioactivity, mostly γ-rays from the ArDM detector materials and the surrounding rock. This article describes the DArT in ArDM project, including the chamber design and construction, and reviews the background required to achieve the expected performance of the detector.

Pacific Northwest National Laboratory (PNNL) has developed a unique fieldable 37Ar measurement system designed to measure 37Ar 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-m3 whole-air samples in 24 h and can measure the 37Ar 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/m3 of 37Ar 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.

This project investigated the feasibility of analyzing radioxenon samples in much larger quantities than currently used by the International Monitoring System (IMS). There is interest within the PTS and the international community in the ability to obtain xenon samples using the output of industrial oxygen plants, which could provide samples that are larger by three orders of magnitude, or more, than those currently provided by IMS stations. Such samples would best be analyzed using internal-source gas proportional counters, though the details of that approach and its sensitivity and limits were previously not examined. This report details the outcomes of a task designed to 1) analyze xenon radioisotope data collected previously via internal-source gas proportional counting and 2) collect additional gas proportional counter measurements to determine feasible gas blends for large volume xenon.

As part of an underground gas migration study, two radioactive noble gases (37Ar and 127Xe) and two stable tracer gases (SF6 and PFDMCH) were injected into a historic nuclear explosion test chimney and allowed to migrate naturally. The purpose of this experiment was to provide a bounding case (natural transport) for the flow of radioactive noble gases following an underground nuclear explosion. To accomplish this, soil gas samples were collected from a series of boreholes and a range of depths from the shallow subsurface (3 m) to deeper levels (~160 m) over a period of eleven months. These samples have provided insights into the development and evolution of the subsurface plume and constrained the relative migration rates of the radioactive and stable gas species in the case when the driving pressure from the cavity is low. Analysis of the samples concluded that the stable tracer SF6 was consistently enriched in the subsurface samples relative to the radiotracer 127Xe, but the ratios of SF6 and 37Ar remained similar throughout the samples.

The measurement of Ar-37 has been proposed as a method of detecting underground nuclear testing. The isotope Ar-37 is generated by neutron activation of calcium by the reaction, Ca-40(n, a)Ar-37, and, as a noble gas, is able to migrate more freely underground. Pacific Northwest National Laboratory has developed a high throughput Ar-37 collection and measurement system using modified Ultra-Low Background Proportional Counters (ULBPCs). This system is capable of collecting, purifying, and measuring radioactivity in argon from either atmospheric or soil gas samples. This process is automated, with minimal operator intervention. This paper describes quantification of Ar-37 and how we account for varying background conditions. An example is provided in which Ar-39 has been shown to be a significant background in some sample sets, created by process K-39(n,p)Ar-39 during an underground nuclear explosion that would also create Ar-37. To account for the large background of Ar-39, we fit the data with a constant plus exponential background model with Gaussian signal model and use the results of a constrained fit to calculate Ar-37 activity. We discuss the methods used to purify and count samples. We discuss the impact of increased Ar-39 backgrounds on the measurement of Ar-37.

This report details the application of neural networks to a data challenge in the classification of pulses generated by an ultra-low background proportional counter (ULBPC) developed at Pacific Northwest National Laboratory (PNNL). In addition to true radioactive decay events there can be spurious pulses detected due to baseline noise, microdischarge, and pileup events. In order to distinguish these events, we leveraged the ability of neural networks to make fine distinctions between inputs. We find that a fully-connected neural network is able to properly classify events in datasets with significant microdischarge and noise contributions.

Building on the successful experience in operating the DarkSide-50 detector, the DarkSide Collaboration is going to construct DarkSide-20k, a direct WIMP search detector using a two-phase Liquid Argon Time Projection Chamber (LAr TPC) with an active (fiducial) mass of 23 t (20 t). This paper describes a preliminary design for the experiment, in which the DarkSide-20k LAr TPC is deployed within a shield/veto with a spherical Liquid Scintillator Veto (LSV) inside a cylindrical Water Cherenkov Veto (WCV). This preliminary design provides a baseline for the experiment to achieve its physics goals, while further development work will lead to the final optimization of the detector parameters and an eventual technical design. Operation of DarkSide-50 demonstrated a major reduction in the dominant 39Ar background when using argon extracted from an underground source, before applying pulse shape analysis. Data from DarkSide-50, in combination with MC simulation and analytical modeling, shows that a rejection factor for discrimination between electron and nuclear recoils of \(>3 \times 10^{9}\) is achievable. This, along with the use of the veto system and utilizing silicon photomultipliers in the LAr TPC, are the keys to unlocking the path to large LAr TPC detector masses, while maintaining an experiment in which less than \(< 0.1\) events (other than \(\nu\)-induced nuclear recoils) is expected to occur within the WIMP search region during the planned exposure. DarkSide-20k will have ultra-low backgrounds than can be measured in situ, giving sensitivity to WIMP-nucleon cross sections of \(1.2 \times 10^{-47}\) cm2 (\(1.1 \times 10^{-46}\) cm2) for WIMPs of 1 TeV/c2 (10 TeV/c2) mass, to be achieved during a 5 yr run producing an exposure of 100 t yr free from any instrumental background.

The Comprehensive Nuclear-Test-Ban Treaty, which is intended to prevent nuclear weapon test explosions and any other nuclear explosions, includes a verification regime, which provides monitoring to identify potential nuclear explosions. The presence of elevated 37Ar is one way to identify subsurface nuclear explosive testing. However, the naturally occurring formation of 37Ar in the subsurface adds a complicating factor. Prediction of the naturally occurring concentration of 37Ar can help to determine if a measured 37Ar concentration is elevated relative to background. The naturally occurring 37Ar background concentration has been shown to vary between less than 1 mBq/m3 to greater than 100 mBq/m3 (Riedmann and Purtschert, 2011). The purpose of this work was to enhance the understanding of the naturally occurring background concentrations of 37Ar, allowing for better interpretation of results. To that end, we present and evaluate a computationally efficient model for predicting the average concentration of 37Ar at any depth under transient barometric pressures. Further, measurements of 37Ar concentrations in samples collected at multiple locations are provided as validation of the concentration prediction model. The model is shown to compare favorably with concentrations of 37Ar measured at multiple locations in the Northwestern United States.

A radiotracer gas with a blend of 37Ar and 127Xe was created for a gas migration experiment and was characterized at Pacific Northwest National Laboratory using ultra-low-background proportional counters. This paper describes the direct low-energy measurement of 37Ar and 127Xe in a dual-isotope sample. Using this low-energy technique, the dual-isotope radiotracer gas was determined to have activity concentrations of 483 Bq/cc and 1435 Bq/cc for 37Ar and 127Xe, respectively, and a ratio of 1:3 on the reference date of 7/11/2016.

Pacific Northwest National Laboratory has accumulated years of data with ultra-low-background proportional counters collected in an on-site shallow underground laboratory. This large dataset of events is exploited to study the impact of using neural networks for data analysis compared to simple pulse shape discrimination (PSD). The PSD method can introduce false positives for overlapping event distributions; however, a neural network can separate and correctly classify these events. This paper describes the training, testing, and validation of a neural network, analysis of challenge datasets, and a comparison between the standard PSD approach and a dense, fully-connected neural network.