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Measurable radiation levels around individuals externally contaminated by nuclear fallout

During the early response to large-scale radioactive contamination events, people who are potentially affected need to be screened for radioactive contamination and public health staff need to triage individuals who may need immediate decontamination. This is typically done by screening individuals for external contamination using ionising radiation detection equipment. In this study, spatially and temporally dependent isotopic compositions from a simulated nuclear detonation and Monte Carlo methods were used to relate contamination activity levels to the measurable radiation levels at select distances away from an individual with whole-body contamination. Radionuclide-specific air kerma rate coefficients and Geiger–Mueller instrument response coefficients at five select distances from contaminated individuals are presented for 662 radionuclides. Temporally and spatially dependent incident-specific coefficients are presented for a hypothetical surface detonation of a 235 U-fueled device.

61 RADIATION PROTECTION AND DOSIMETRY↗

Biofilm growth in water-cooling towers as collection platforms for airborne radionuclides

Given its history of nuclear material processing, the Savannah River Site (SRS) was used to evaluate whether biofilms growing in water-cooling towers (WCTs) are effective passive collection platforms for environmental radionuclide surveillance. Uranium and plutonium analyses suggest that WCT-sourced biofilms are efficient, indigenous, constantly running samplers that can be used for environmental monitoring, as their isotopic compositions are distinct from atmospheric fallout and representative of SRS historical activities. Further, the ubiquity of WCTs worldwide and demonstrated ability to detect nuclear material processing and constrain specific activities based on biofilm actinide isotopic compositions make WCT biofilms a promising means to improve monitoring.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Development and testing of a fission-like neutron field for dosimetry and instrument calibrations based on deuterium-tritium generator

For nearly five decades 252 Cf sources have been used for testing and calibration over a wide range of neutron detection devices used for nuclear safety and radiation protection. However, the vastly increased cost of 252 Cf sources, its short half-life, and concerns about future shortage have prompted nuclear facilities and radiological calibration laboratories that rely on high-intensity neutron sources to seek alternatives. There appear to be no other radionuclide neutron sources that would match “like-to-like” 252 Cf performance characteristics. Alternatives of producing a fission-like neutron spectrum based on commercially available deuterium-tritium (D-T) generators, and without any fissionable materials or beryllium, have been explored. This paper describes efforts of designing the spectrum shaping assembly, its construction and installation. The produced neutron field was evaluated both from the perspective of the neutron fluence spectrum and the resulting dosimetric outcome. Finally, it was tested for practical application by examining response of various health physics instruments and personal monitoring devices in comparison to the response of those devices when exposed to 252 Cf. In conclusion, the response of survey-type instruments tested within the prototype, surrogate fission, reference field are acceptably close to their response in the targeted 252 Cf field.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A Fission-like Neutron Spectrum Shaping Assembly based on D-T Generator

For nearly five decades, 252 Cf sources have been used for testing and calibration over a wide range of neutron detection devices used for nuclear safety and radiation protection. However, the vastly increased cost of 252 Cf sources, its short half-life, and concerns about future shortage have prompted nuclear facilities and radiological calibration laboratories that rely on high-intensity neutron sources to seek alternatives. While there appear to be no other radionuclide neutron sources that would match the 252 Cf performance characteristics, all of them, including 252 Cf, present similar concerns in terms of hazards, safety, and security. As a possible solution to this issue, the Pacific Northwest National Laboratory (PNNL) developed a low-risk, cost-efficient alternative to produce fission-like spectra based on commercially available deuterium-tritium (D-T) neutron generators. The alternative of producing a fission-like neutron spectrum without any fissionable materials or beryllium would enable the nuclear facilities across the entire complex to eliminate their reliance on high intensity 252 Cf sources for nuclear safety and radiation protection applications, substantially reducing risks and associated costs. This report describes efforts of designing the spectrum shaping assembly, its construction and characterization of the neutron field produced. Performance of this newly developed D-T generator based neutron field is demonstrated via calibration of a criticality detector, neutron survey instruments, and personal dosimeters verified against current standardized fields produced by 252 Cf spontaneous fission sources.

42 ENGINEERING↗

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

The development of measurement methodologies to detect and monitor nuclear-relevant materials remains a consistent and significant interest across the nuclear energy, nonproliferation, safeguards, and forensics communities. Optical spectroscopy of laser-produced plasmas is becoming an increasingly popular diagnostic technique to measure radiological and nuclear materials in the field without sample preparation, where current capabilities encompass the standoff, isotopically resolved and phase-identifiable (e.g., UO and UO[Formula: see text]) detection of elements across the periodic table. These methods rely on the process of laser ablation (LA), where a high-powered pulsed laser is used to excite a sample (solid, liquid, or gas) into a luminous microplasma that rapidly undergoes de-excitation through the emission of electromagnetic radiation, which serves as a spectroscopic fingerprint for that sample. This review focuses on LA plasmas and spectroscopy for nuclear applications, covering topics from the wide-area environmental sampling and atmospheric sensing of radionuclides to recent implementations of multivariate machine learning methods that work to enable the real-time analysis of spectrochemical measurements with an emphasis on fundamental research and development activities over the past two decades. Background on the physical breakdown mechanisms and interactions of matter with nanosecond and ultrafast laser pulses that lead to the generation of laser-produced microplasmas is provided, followed by a description of the transient spatiotemporal plasma conditions that control the behavior of spectroscopic signatures recorded by analytical methods in atomic and molecular spectroscopy. High-temperature chemical and thermodynamic processes governing reactive LA plasmas are also examined alongside investigations into the condensation pathways of the plasma, which are believed to serve as chemical surrogates for fallout particles formed in nuclear fireballs. Laser-supported absorption waves and laser-induced shockwaves that accompany LA plasmas are also discussed, which could provide insights into atmospheric ionization phenomena from strong shocks following nuclear detonations. Furthermore, the standoff detection of trace radioactive aerosols and fission gases is reviewed in the context of monitoring atmospheric radiation plumes and off-gas streams of molten salt reactors. Finally, concluding remarks will present future outlooks on the role of LA plasma spectroscopy in the nuclear community.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Evaluation of Naturally Occurring Be-7 Activity on LANL Stack Filter Clumps

Los Alamos National Laboratory (LANL) is responsible for providing solutions to challenging issues through multidisciplinary science, engineering, and technology that impact national security. As part of the Radioactive Air Emissions Management (RAEM) Team, it is our responsibility to ensure LANL operates within the requirements of the Code of Federal Regulations 40 CFR 61, Subpart H, National Emission Standards for Emissions of Radionuclides Other Than Radon From Department of Energy Facilities (Rad-NESHAP). The standard states, “Emissions of radionuclides to the ambient air from Department of Energy facilities shall not exceed those amounts that would cause any member of the public to receive in any year an effective dose equivalent of 10 mrem/yr” (EPA, 2002) During a routine assessment of LANL’s Rad-NESHAP compliance program, an opportunity for improvement was identified that addresses the evaluation of routine stack samples which potentially have naturally occurring radioactive materials (NORM) on the filter media. In the past and based on professional judgment, detections of NORM such as K-40 and Be-7 typically were rejected from the analytical results. The assessment finding suggested developing a technical criterion to ensure that such rejections were justified, comparing actual measured values with anticipated NORM concentrations for various stacks located at LANL. The significance of accepting or rejecting samples as “true” or “NORM” and its impact on the RAEM’s mission and compliance to the regulations is explained later in the document. Additionally, this document will describe the process and calculations for how such results are to be accepted as actual samples “true positive” or rejected as NORM.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Nuclear Forensics National Frameworks [Slides]

Nuclear forensics is the examination of nuclear or other radioactive material, or of evidence contaminated with radionuclides, in the context of legal proceedings under international or national law related to nuclear security. The goal of forensic science is to discover linkages among people, places, materials, and events. Nuclear forensics is an essential component of national response plans to events involving nuclear or other radioactive materials out of regulatory control and informs prevention, detection, and response.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Investigation Support Scenario-based Policy Discussion Development [Slides]

Nuclear forensics is the examination of nuclear or other radioactive material, or of evidence contaminated with radionuclides, in the context of legal proceedings under international or national law related to nuclear security. The goal of forensic science is to discover linkages among people, places, materials and events. Nuclear forensics is an essential component of national response plans to events involving nuclear or other radioactive materials out of regulatory control and informs prevention, detection and response.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Summary of Analytical Results from Samples Supporting Tank Closure Cesium Removal (TCCR) Batch 3 and Modeling Results for Cs Loading on CST

Savannah River Remediation (SRR) is currently operating the Tank Closure Cesium Removal (TCCR) process to remove 137 Cs from tank waste supernate using an ion exchange process. As part of that process, Savannah River National Laboratory (SRNL) receives and analyzes samples in support of the qualification of each batch to be processed. SRNL recently received supernate samples retrieved from Tank 10H as well as in-tank batch contact samples for characterization in support of qualifying Batch 3 for processing through the TCCR unit. Some results from analysis of those samples have been previously reported. This report documents the remaining analyses of the in-tank batch contact samples as well as the results of ZAM (Zheng, Anthony, Miller) isotherm modeling performed for comparison to the measured results. Results of the additional analyses include analysis of the loading of other radionuclides besides 137 Cs on the crystalline silicotitanate (CST) contained within the in-tank batch contact test samples. Results from those analyses revealed the next highest contributor to the activity on the CST was 90 Sr with an average loading of 2.76E+08 dpm/g CST compared to 3.56E+10 dpm/g CST for the 137Cs. Isotopes of plutonium were also detected on the samples. ZAM modeling was performed using the measured composition of the Tank 10H Batch 3 qualification samples. The modeling predicted a maximum Cs loading approximately 2.2x higher than the measured result. This is a slightly lower ratio (expected/measured) compared to what was observed for the prior TCCR in-tank batch contact testing performed for Batches 1A and 2 where the ZAM results were 2.7-2.8x higher than the measured values.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Inverse aqueous transport modeling for emergency response

ALGE is a three-dimensional, finite-difference aqueous transport model that simulates pollutant fate and transport in lakes, rivers, bays, and estuaries by solving the prognostic equations of mass, momentum, and energy. Its current modeling capabilities include transport of dissolved tracer for a series of predefined basins across the continental United States. Recently, an inverse method (also known as backtracking) has been added to ALGE to provide a possible source of a pollutant should one be detected by a sensor in a body of water and a source is not known. This inverse method is a three step process that uses an algorithm to inverse the flow. We demonstrate the new model’s capabilities through simulating the 2021 Piney Point spill in Tampa Bay, Florida (USA). This involves moving tracer backwards from its detection points, encompassing a potential source area, and applying Bayes’ Theorem and $\frac{𝜒}{𝑄}$ to reduce the area within which the true source could be located.

hydrological modeling↗

A comparison of long-term 37 Ar and 39 Ar transport and implications for 39 Ar as a persistent indicator of underground nuclear explosions

Measurements were first made in 2016 of legacy 39 Ar gas from the decades-old Barnwell underground nuclear explosion site within the Nevada National Security Site. This has raised the question of the ubiquity of the radionuclide 39 Ar following underground nuclear explosions in general locations. This article presents a high-level evaluation of the scientific case for using 39 Ar as a long-term indicator of underground nuclear explosions. Assessment is made based on a broad set of assumptions to reasonably estimate the persistence of 39 Ar in the subsurface environment following an explosion to establish potential detectability years to decades after the originating event.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Measurements of radioxenon activities during periods of gaseous release from an advanced gas-cooled reactor

Activities of radioxenon isotopes are reported from an Advanced Gas-cooled Reactor (AGR) during periods of gaseous release. Xenon isotopes are relevant to the monitoring regime of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). These releases may affect detections from the International Monitoring System (IMS) by influencing the radioxenon background. Time series activity plots have been produced from both in-core monitoring and direct measurement at the point of release using a stack monitor system. Ratio plots using both data sets have been produced with results compared with a commonly chosen nuclear explosion “discrimination line.” The reported results improve the understanding of radionuclide emissions from civil nuclear power plants. This work is being performed as part of the Xenon Environmental Nuclide Analysis at Hartlepool (XENAH) collaboration between the Atomic Weapons Establishment (AWE, UK), EDF Energy (UK), Pacific Northwest National Laboratory (PNNL, USA), and the Swedish Defence Research Agency (FOI).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Cerium oxide impact on fresh and hardened properties of cementitious materials

Cements used in global nuclear waste treatment, storage, and disposal require thorough testing of fresh and cured properties to demonstrate regulatory compliance. Using actual radioactive wastes is often cost-prohibitive during early scoping tests necessitating the use of non-radiological surrogates. Cerium (Ce) is often used as a surrogate for actinides uranium (U) and plutonium (Pu) in spent nuclear fuel, yet few studies have explored how Ce impacts the properties used to qualify a cement for use. Here, this work compares the fresh and cured properties of three classes of cements – ordinary portland cements, ultra-high performance cement composites, and magnesium phosphate cements – each with and without ceria (CeO 2 ). Due to CeO 2 sorption of water (54 vol%) that effectively decreases the water available to hydrate and form binding cement phases, variations in key cement properties were detected that suggest surrogate CeO 2 –cementitious matrices may not be representative of matrix behaviors when using U and Pu sources.

36 MATERIALS SCIENCE↗

URINARY EXCRETION OF PLUTONIUM IN MAYAK WORKERS DURING AND AFTER CA-DTPA ADMINISTRATION

Chelation therapy is sometimes used after potential exposures to plutonium to increase urinary excretion of the radionuclide to improve the accuracy of bioassay measurements. The purpose of this report is to describe the enhancement of urinary excretion of plutonium during and after the administration of the trisodium salt of calcium diethylenetriaminepentaacetate (Ca-DTPA) daily for 3 d to a group of male and female plutonium workers from the Mayak Production Association in Ozyorsk, Russia. One-hundred and two cases (18 females and 84 males) were selected where urinary contents of plutonium, prior to chelation, exceeded the detection threshold. Daily urine collections were obtained during the 3 d of Ca-DTPA treatments. In addition, 58 of these cases had urine bioassays at 1–45 d after chelation. The daily enhancement over baseline values excretion of plutonium was found to be 50.4×/1.4 (geometric mean and geometric standard deviation); 58.9×/1.2; 72.9×/1.4 in the first, second and third days of Ca-DTPA administration. The mean enhancement for the 3-d period was 60.1×/1.7. The rate of plutonium excretion from 1 to 45 d after chelation decreased with a half-period of 3.9 d and the chelation enhancement factor (Кenh-i) is described by the function Кenh-i = (0.79 ± 0.24) + (42.9 ± 1.2) × e-(0.18 ± 0.01) × day.

Environmental Sciences & Ecology↗

Application of Indirect Quantification of 133mXe to Calibration of HPGe Detector

The INL Noble Gas Laboratory provides intercomparison samples for the noble gas analysis laboratories as part of the CTBTO PrepCom IMS. Xe-133m is one of the four relevant radionuclides in nuclear explosion monitoring. Without commercially available Xe-133m calibration standards laboratories must create and improve calibration methods. Improvements in calibration methods at the INL NGL benefit the CTBTO PrepCom through better certified values for Xe-133m intercomparison samples. Calibration of High Purity Germanium detectors for Xe-133m quantification is complicated by the coexistence of Xe-133 in samples under analysis. Xe-133 is typically produced in larger quantities, has higher gamma emission probabilities, and its gammas are detected more efficiently than Xe-133m. Xe-133m activity of samples can be indirectly inferred through the 133:133m activity ratio of a batch of material, and the Xe-133 counts in the assay of a small aliquot of the same material. This indirect quantification method can be leveraged to perform detector calibrations for quantification of Xe-133m. Calibrations can be performed by inferring the Xe-133m to certify the sample, and direct counting to determine detector efficiency. A comparison of method results will be shown.

133mXe↗

Characterization of Tank 9H Annulus Sample in Support of Residual Material Inventory Determinations

The Savannah River National Laboratory (SRNL) was requested by Savannah River Mission Completion (SRMC) to provide sample preparation and characterization of the Tank 9H annulus sample in support of Residual Material Inventory Determinations. One Tank 9H sample in three vials [HTF-9-25-13, HTF-9-25-14 and HTF-9-25-15], with each vial containing approximately 200 mL of the Tank 9H annulus salt solution, were delivered to the SRNL Shielded Cells for sample preparation and characterizations in February 2025. The density of the “as-received” solution contained in each of the three Tank 9H annulus sample vials were determined followed by a solid-liquid separation on each one using 0.45-micron Nalgene® nylon filter membranes. The resulting filtrates were combined to form the Tank 9H annulus sample with a total volume of about 600 mL. The combined wet solid fractions, about a total of 4.8 grams of salt material, remaining on the filter membranes were air-dried in the Shielded Cells for 72 hours. The total weight of the air-dried solids was 2.1 grams. These air-dried solids were washed with deionized water (DI water) at a phase ratio of 60 mL DI water/gram of solids to recover insoluble solids, if any. No visible or measurable quantity of insoluble solids were recovered after DI water washing of the air-dried solids because the air-dried solids completely dissolved in the DI water. The solid fraction-wash water was not combined with the 600 mL of the filtrate solution, and the resulting solution was not screened or analyzed for radionuclides. Aliquot sample volumes of the undiluted Tank 9H annulus sample were sent to the SRNL analytical services groups for radionuclides, elementals, anions and total mercury analysis by various methods including radiochemical separations/counting methods, inductively coupled plasma-atomic emission spectroscopy (ICP-AES), and Inductively Coupled Plasma Mass Spectroscopy (ICP-MS) and special preparations. All sample analyses were performed in triplicate. This report presents the analytical characterization results for the Tank 9H annulus sample. The results are also reported where analytical methods yielded additional analytes, other than those requested by SRMC. In the characterization of the Tank 9H annulus sample, the detection limits for all the analytes, as specified in the Technical Task Request (TTR) and Task Technical and Quality Assurance Plan (TTQAP), were met.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Analysis of measurements from an array of radioxenon samplers near to Hartlepool Nuclear Power Station

As part of a scientific research and development project, the radionuclide fingerprint of an operating advanced gas-cooled reactor 25 (AGR) has been studied across several facets (Goodwin et al., 2024). One part of this project was to deploy an array of 26 radioxenon samplers to the region for a period of around 1 year, to measure any radioxenon emissions from the reactors of the 27 Hartlepool nuclear power station at a range of tens of kilometres away. The array of 3 sensors was operational for around 12 28 months from March 2022 and detected many occurrences of isotopes of radioxenon. Here we provide a detailed analysis and 29 interpretation of the data and where possible, attribution of detections to a source or region. Whilst a key part of this work is to 30 measure any emissions of radioxenon from Hartlepool, this work presents one of the most comprehensive efforts to determine the 31 source of a great number of (mostly) 133Xe detections. A combination of different types of atmospheric dispersion modelling 32 techniques, including the use of stack monitoring data from nearby civil radioxenon-emitting nuclear facilities has enabled the 33 majority of detections to be attributed to one or more possible sources. Whilst emissions from Hartlepool have been detected on 34 the systems, the majority of detections are associated with a medical isotope production facility in Fleurus, Belgium (IRE).

Advanced gas-cooled reactor↗

Colloid-Facilitated Actinide Transport in a Cementitious-Impacted SRS Groundwater

The objective of this report is to provide a literature review relevant to the question of whether colloid facilitated transport of plutonium is enhanced in a cementitious groundwater system on the Savannah River Site (SRS). Contaminant transport is commonly described as taking place in a system with a mobile aqueous phase and an immobile solid phase. There has been an increasing awareness of a third phase, a mobile solid phase, also referred to as a mobile colloidal phase. Mobile colloids consist of organic and/or inorganic submicron-particles that move with groundwater flow. When radionuclides are associated with the mobile colloids, the net effect is that radionuclides can move faster through the subsurface system than would be predicted by transport models that do not include mobile colloids. It is important to distinguish between subsurface colloids and subsurface mobile colloids. The subsurface environment includes an enormous reservoir of colloids, but only a tiny fraction, if any, are mobile. Mobile colloid formation is commonly described as involving a three-step process: genesis, stabilization, and transport. It was concluded that there is a strong likelihood that submicron colloids of plutonium exist near the source term, (i.e., the genesis step is likely completed). While such particles have not been directly detected, it is highly likely that plutonium could either attach to submicron particles in the sediment or that submicron plutonium fragments exist at the source. However, the tendency for these plutonium colloids to move in the SRS subsurface is extremely low, especially in engineered cementitious environments where the ionic strength of the solution and the elevated concentrations of divalent cations greatly curtails colloid suspension stability (i.e., the stabilization step is likely not completed). Together these data strongly indicate that plutonium-bearing colloids would likely exist in the near field of a tank closure facility, but the colloids would be unlikely to be mobile, thereby providing a vector for enhanced transport. Under cementitious leachate impacted groundwater conditions, it is reasonable to assume plutonium transport occurs primarily as a two-phase system, a mobile aqueous phase and an immobile solid phase.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗