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A Review of the Lawrence Livermore Nuclear Accident Dosimeter 1980s-present

A Nuclear Accident Dosimetry program is a federal requirement for all facilities that have the potential to have a criticality accident. Personnel Nuclear Accident Dosimeter (PNAD) theory and analytical procedures are driven by various scientific needs and interacting regulations. A brief history of the status of USA Department of Energy (DOE) nuclear accident dosimetry regulations, recommendations, and performance testing criteria are given. Then, the history of the Lawrence Livermore National Laboratory (LLNL) PNAD is explored, including changes in the physical dosimeter and adjustments of the analysis method through the last four decades. Finally, the performance of LLNL’s PNAD at criticality accident intercomparison training exercises since 2009 is explored. In general, reported neutron doses have been within or close to DOE-STD-1098 performance criteria while reported gamma doses have been outside of DOE-STD-1098 performance criteria. Reported total absorbed doses have varied in meeting ANSI/HPS N13.3 and ANSI/HPS N13.3 (R2019) performance criteria. Dosimetry staff retirement and turnover have left historical knowledge gaps, yet provided opportunities within the NAD program at LLNL. This review paper serves as an overview of the history and status of the NAD program. Brief technical, procedural and programmatic recommendations to improve LLNL’s NAD program are given. Technical recommendations include investigating orientation factors through modeling or empirical experimentation, investigating gamma dosimetry methods for high-dose scenarios, and exploring other dosimetric methods for simpler, quicker NAD analysis. Procedural recommendations include better documentation of conversion factor (activity-to-fluence and fluence-to-dose) derivations and spectrum uses, and updated analysis spreadsheets or simple Graphic User Interfaces for dose calculations. In conclusion, programmatic recommendations include formalized training for NAD analysts, and having multiple SMEs trained on the NAD program.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Universal Nuclear Accident Dosimeter

The Lawrence Livermore National Laboratory (LLNL) Universal Nuclear Accident Dosimetry (UNAD) project is a four-year initiative aimed at advancing nuclear accident dosimetry methods. This article presents an overview of the research, key findings, and the progress made throughout the project. The primary goals included a background into the history of nuclear accident dosimetry, consolidating current dosimetry techniques within the NNSA/DOE complex, fostering collaboration among subject matter experts, and exploring novel technologies for potential implementation. The technical focus centered on investigating new and novel technologies, instrumentation methods, and analysis methods to develop recommendations for a potential nuclear accident dosimeter (NAD) to be universally deployed through the DOE complex. A multilaboratory and multinational Usergroup was established, conducting periodic meetings to facilitate knowledge exchange. The UNAD team has participated in two international nuclear accident dosimetry intercomparison exercises and one characterization exercise, where the existing LLNL NAD and a prototype alanine electron paramagnetic dosimeter NAD were deployed. Ongoing improvements are being made to the prototype NAD based on results from the exercises, laboratory studies, and collaboration with other laboratories. A machine learning algorithm to optimize the geometry and conversion factors of the current LLNL NAD is being implemented, and the resulting design will be tested in the next exercise. In conclusion, key lessons learned and future directions for the project are discussed.

Electron paramagnetic resonance spectroscopy

Fading study of Harshaw LiF:Mg,Ti thermoluminescence dosimeters exposed to neutron doses

Sensitivity and signal fading were tested in Harshaw LiF:Mg,Ti thermoluminescence dosimeters (TLDs) exposed to neutron and beta/photons doses. A significant difference in the signal fading rate was observed for TLDs exposed to neutrons compared with TLDs exposed to betas. This difference may have been related to differences in glow curves for dosimeters exposed to different beams and to differences in glow curve evolution after exposure. A fading-correction algorithm was developed to correct the cumulative sensitivity + signal fading of TL doses for the fading time t using the formulae: y = 0.147∗exp(-t/4.36) + 0.308∗exp(-t/34.1) + 0.73 for neutrons, and: y = 0.132∗exp(-t/10.72) + 0.174∗exp(-t/31.5) + 0.8 for betas/photons. The formula was validated using the dose recovery test, where the average deviation of fading-corrected doses from delivery doses was within 1%. In conclusion, the proposed fading-correction approaches may significantly improve the accuracy of Harshaw TL dosimetry with LiF:Mg,Ti cards for both neutron and beta/gamma irradiation.

61 RADIATION PROTECTION AND DOSIMETRY

Implementation of Stochastic Gradient Descent in an Automated Glow Peak Identification Software for Multiple Thermoluminescent Dosimeter Types

A glow-curve analysis code was previously developed in C++ to analyze thermoluminescent dosimeter glow curves using automated peak detection while applying a first-order kinetics model. A newer version of this code was implemented to improve the automated peak detection and curve fitting models. The Stochastic Gradient Descent Algorithm was introduced to replace the prior approach of taking first and second-order derivatives for peak detection. Additionally, early stopping mechanisms were invoked to improve the previously used Levenberg-Marquardt Algorithm employed for curve fitting. The two software versions were compared through glow curve analysis of different thermoluminescent dosimeter materials and calculation of the corresponding figures of merit. Altogether improvements were shown, namely an increase in the number of peaks detected and a reduction of the mean figure of merit by approximately 46%.

137Cs

A Novel Dosimetry Method for Small Animal Irradiators Using 3D-printed Mouse Phantoms and Alanine Dosimeters

Abstract Accurate dosimetry is a crucial component of small animal and preclinical irradiation studies. Various dosimetry options are available but fail to characterize complex geometries and variable energy spectra of modern x-ray irradiators accurately. These options also lack national/international standards of recognition. This paper presents a novel dosimetry system, Dosequate, which uses murine phantoms embedded with alanine dosimeters and paired with x-ray energy spectra corrections to deliver consistent and accurate dosimetry measurements. This study compares Dosequate measurements against a Precision X-RAD 320 internal ion chamber and the treatment planning system of an Xstrahl Small Animal Radiation Research Platform. Results demonstrate the accuracy and reproducibility of the Dosequate system, highlighting its potential for standardizing dosimetry in preclinical research throughout the industry. Results demonstrate the accuracy and reproducibility of the Dosequate system, highlighting its potential for standardizing dosimetry in preclinical research throughout the industry. The Dosequate dosimetry method provides a robust and standardized approach for measuring absorbed dose in small animal irradiators. Its accuracy, reproducibility, and ability to account for complex irradiation geometries make it a valuable tool for preclinical research. This system has the potential to significantly improve the intercomparability of studies across different facilities and enhance the reliability of results.

Environmental Sciences & Ecology

Directional dependence of equilibrated TLD-400 chips in multiple radiation fields

Fielding of thermoluminescent dosimeters (TLDs) for measurement of photon radiation dose in experiments is the standard practice for γ-irradiation facilities, pulsed power x-ray facilities, and reactor facilities at Sandia National Laboratories (SNL). Due to the high-dose experimental conditions and the mixed ( 1 n, γ) fields in these facilities, SNL radiation metrologists have historically used CaF 2 :Mn TLDs (also known as TLD-400). Recent inquiries to the radiation metrology staff have raised concerns that the aluminum-equilibrated TLD-400 chips may exhibit a directionally dependent response. The metrologists were asked whether the dose measured by the chip may be impacted by the angle of incidence on the equilibrated TLD. To provide a thorough answer to this query, a set of adjoint Monte Carlo radiation transport calculations was performed for three different equilibrated TLDs as well as bare TLD chips using the Integrated Tiger Series (ITS) code. The key feature of the adjoint calculations performed in this study is that each photon escaping the modeled geometry was tallied into angular bins to provide information on both the energy and angular dependence of the equilibrated chip. After the adjoint Monte Carlo calculations were completed, the resulting energy-dependent response function for each angular bin was convolved with multiple photon energy spectra representing various radiation facilities at SNL. The radiation facilities selected for analysis span a range of photon energies from approximately 1 keV up to approximately 20 MeV. Thus, the presented results are applicable to a wide variety of radiation facilities around the world. Although the bare TLD-400 chip was expected to display the largest variation due to the photon angle of impact on the dosimeter, the dosimeter with the thinnest aluminum equilibrator (SNL thin equilibrated TLD-400) was determined to have the biggest differential between the impact angle with the maximum dose ( D max ) and the impact angle with the minimum dose ( D min ). However, the SNL normal equilibrated TLD-400 chip demonstrated a dramatic reduction in that differential between maximum and minimum dose angles. The reduction in this differential is one of the dominant factors in experimenters’ choice to field these dosimeters at SNL radiation facilities. The results from the PNNL (Hanford) energy-flattening field capsule are consistent with the previous publications. The differential dose responses due to the photon impact angle indicate that experimenters should strive to field their TLD-400 dosimeters in a consistent manner to avoid additional uncertainty in the measurements based on dosimeter orientation.

Adjoint radiation transport

A review of criticality dosimetry at the Y-12 National Security Complex and practical importance of dose accuracy in emergency response

A nuclear criticality results in the emission of both neutron and gamma radiation and can produce doses to personnel near the event that exceed 0.1 Gy (10 rad). The primary purpose of nuclear accident dosimetry is to rapidly identify affected personnel in need of prompt medical treatment and to reassure personnel who have been only minimally exposed. While accurate dosimetry is desired, it must be recognized that dose determinations made from whole-body dosimeters or simple triage methods are very rough estimates and contain significant uncertainties. Even when accounting for factors like varying neutron energy spectra, mean photon energies, body orientation within the radiation field, and transient effects on dosimeter response, etc., the end value is a dosimetric quantity defined for very specific radiological conditions and determined within a simple phantom usually at a single depth. Of more importance is the biological response to the radiation, which will vary by person and can be affected by the individual’s radiation sensitivity, age, gender, mass, and underlying health conditions. The overall biological, person-specific response to a given dose cannot be precisely determined except by patient symptom observation and individual biological dosimetry (e.g. chromosome analysis, lymphocyte ratios, etc.). This work describes and discusses the criticality accident dosimetry program at the Y-12 National Security Complex, a United States Department of Energy National Nuclear Security Administration facility. In conclusion, the primary goals of the Y-12 accident dosimetry program are, among others, the rapid identification of significantly exposed persons, prompt routing of exposed workers for medical evaluation and treatment, and the ultimate processing of dosimeters to assign doses to personnel.

61 RADIATION PROTECTION AND DOSIMETRY

Fabrication and Testing of Micro Flux Monitors in the High Flux Isotope Reactor

Neutron dosimetry is a critical technique to measure the neutron flux, fluence, and energy spectrum of nuclear reactors and can be used to indicate fuel reloading, high-power operations, or changes in cycle length. This work presents results of a novel device named the micro flux monitor, which is a miniaturized neutron dosimeter made from small quantities (100s of nanograms) of Ti, Al, Ni, and Au metals deposited on Si and high-purity fused silica substrates using standard semiconductor fabrication techniques. Approximately 1,250 of these devices were produced, and 40 were irradiated in the pneumatic tube facility of the Neutron Activation Analysis Laboratory at the High Flux Isotope Reactor. Testing demonstrated that dosimeter metals can be deposited predictably and repeatedly in multiple geometries, including as quick response (QR) codes. Neutron flux measurements with these devices were within 3% of measurements made using standard flux monitors, demonstrating the efficacy of these devices. Devices were also tested at 500°C under a N2 atmosphere and showed minimal degradation, suggesting they could be deployed for neutron dosimetry measurements in high-temperature advanced reactors.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS

AGC-4 As-Run Uncertainty Analysis

The concept of measuring neutron flux (or fluence rate) with activation foils has existed since the late 1940s and is a well-used methodology. Activation foils are selected for their unique isotopic cross sections that create reaction products with desirable properties: relatively simple radioactive decay scheme, measurable quantities of gamma-rays or betas, and half-lives appropriate for the irradiation and decay durations of the experiment. The activation materials, deemed flux wires, fluence wires, dosimeters, or flux foils, are fabricated to have a mass appropriate for the irradiation as well so the measurement using a radiation detector following the irradiation is sufficient but not overwhelming in terms of total activity. Activation measurement results are expressed in terms of reaction rate, which can then be used to “adjust” the neutron spectrum. The Advanced Graphite Creep (AGC)-4 experiment contained 26 flux wire packages, each containing an iron and a niobium wire inside a vanadium capsule. For all stackup positions, the value of fast to thermal neutrons is higher than expected, but the total neutron fluence is near the predicted value of ~2 x 1022 n/cm2. As compared to the predicted neutron spectrum, there are four takeaways in the results as compared to the predicted ATR irradiation: 1) Additional fast (fission) neutrons present, 2) Spectrum hardening due to temperature, 3) Spectrum hardening due to container attenuation, 4) Total neutron fluence is close to predicted values. Since the neutron energy spectrum is a key parameter when attributing neutron damage in materials, the adjusted energy-dependent spectrum and the total neutron fluence results from the dosimeters can be incorporated for future calculations.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Results of South-East Flux Trap Dosimetry Measurements for the Advanced Test Reactor Critical Facility in support of Advanced Sensors and Instrumentation Development

Reactor dosimetry measurements are commonly used to validate simulation and modeling in nuclear reactor tests. Numerous standard dosimeter materials exist which are commonly utilized with sensitivities to different energy ranges of neutrons. At the Advanced Test Reactor (ATR), cobalt alloy and pure nickel wires are installed every cycle to monitor thermal- and fast-neutron fluence rates. However, there is growing interest in exploring less commonly used materials which are either more sensitive to different parts of the neutron energy spectrum or which can incorporate multiple activation paths in a single material. Epithermal and fast-neutron energies beyond the typical 1-MeV threshold are of particular interest. Two ATR-C Flux Runs took place during 2024; each flux run included supplemental dosimetry packages in the South-East Flux Trap (SEFT) Filler. The focus of the dosimetry package for flux run 23-4 was to test two novel dosimetry methods that can provide simultaneous thermal and threshold (fast) sensitivity in a single dosimeter wire. A selection of 3% Au in Cu alloyed wires were available that provided sensitivity to fast and thermal neutrons through 5 different reactions. Likewise, Fe offers multiple interaction pathways with sensitivity to both thermal and fast neutrons. The main question to be answered by these irradiations was if sufficient radioactivation would take place in the ATR-C SEFT during a nominal 20-minute irradiation at typical power levels (near 600Wth) to observe the threshold reactions that have smaller activation cross-sections than the thermal reactions without being saturated by interfering interactions and Compton continuum during the High-Purity Germanium (HPGe) measurements. The results from comparing the measurement results to anticipated activity levels provide confidence in our ability to activate both traditional and novel dosimetry materials in ATR-C, however not all the measured values matched with the predicted activities. This leaves further room for investigation both on the experimental and computational approaches for future irradiation experiments.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN

Integrating HPC simulations and physical experiments to characterize the effects of gamma radiation on seismic protective devices

Seismic protective systems, composed of seismic isolators and dampers, can substantially reduce the effects of earthquake shaking on nuclear power plants and components therein. To enable the use of these devices to protect equipment inside a plant and close to a source of radiation, the U.S. Department of Energy (DOE) funded a project at the Idaho National Laboratory (INL) and the University at Buffalo to characterize the effects of absorbed gamma dose on their mechanical properties. An early task in the project was to determine the exposure time required in the INL Foss Therapy Services (FTS) 60 Co gamma irradiator to achieve a target absorbed dose in the materials used to construct isolators and dampers, including fluids, polymers, composites, and metals. This task required the novel integration of high-performance computing (HPC), Monte Carlo N-Particle (MCNP) simulations, and irradiation experiments using Fricke dosimetry. An MCNP model of the FTS irradiator at INL was developed and validated using Fricke dosimetry. Simulations of three experiments in the irradiator, two with Fricke vials only and one with Fricke vials and a large-size isolator, predicted the Fricke-measured absorbed dose rate to within 15% in all three cases, providing high confidence in the calculation of the gamma dose absorbed in the materials comprising the seismic protective devices. The simulations demonstrated that the effects of photon scattering on absorbed dose rate in the FTS irradiator are negligible for test articles installed close to the cobalt sources and near the rear of the irradiator. The validated MCNP model of the FTS irradiator is being used to support ongoing DOE-funded experiments on seismic protective devices and could be applied to future, non-seismic-related experiments. In conclusion, the novel validation process successfully deployed for the FTS irradiator at INL could be applied to other irradiators, requiring new MCNP models and simulations, and irradiation experiments using dosimeters.

42 - ENGINEERING

Measuring very low radiation doses in PTFE for nuclear forensic enrichment reconstruction

Every country that has made nuclear weapons has used uranium enrichment to do so. Despite the centrality of this technology to international security, there is still no reliable physical marker of past enrichment in the open literature that can be used to perform forensic verification of historically produced weapons on gas centrifuges. We show that the extremely low radioactivity from uranium alpha emissions during enrichment leaves detectable and irreversible calorimetric signatures in the common enrichment gasket material PTFE, allowing for historical reconstruction of past enrichment activities at a sensitivity better than one weapon’s quantity of highly enriched uranium. Fast scanning calorimetry also enables the measurement of recrystallization enthalpies of sequentially microtomed slices, confirming the magnitude and the type of radiation exposure while also providing detection of tampering and a method for analyzing field samples useful for treaty verification. Furthermore, this work opens the door for common items to be turned into precise dosimeters to detect the past presence of radioactivity, nuclear materials, and related activities with high confidence.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P

A neutron fluence map of the Los Alamos National Laboratory Godiva IV critical assembly

A neutron fluence map and a total ionizing dose map of the Los Alamos National Laboratory Godiva IV fast burst critical assembly was generated using passive reactor dosimetry, comprised of sulfur pellets and thermoluminescent dosimeters. Godiva IV is an unmoderated, fast burst, critical assembly constructed of approximately 65 kg of highly enriched uranium fuel alloyed with 1.5 % molybdenum for strength. The mapping was performed during a single 75.6 ºC temperature rise burst operation, with the top and sides of the cylindrical Godiva-IV Top Hat covered in passive dosimetry. Dosimetry was placed in a symmetric pattern around the Top Hat, with higher concentrations near the control rods and burst rod. A specific portion of the lower quadrant of the burst rod was mapped to confirm a testing region where the neutron fluence varied by no more than ± 5%. The results will be used to assess the neutron, gamma, and total ionizing dose environment in three-dimensional space around the assembly for higher fidelity experiment placement, active dosimetry positioning, and radiation field characterization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Reconstructing Hanford worker external doses from photons for epidemiology

The accurate reconstruction of external photon doses is essential for credible radiation epidemiology. This article presents the methodology used to derive dose estimates for 37 012 Hanford Site workers included in the Million Person Study. The approach employs historical dose records from the Hanford Radiation Exposure database and a previous epidemiology study. Bias correction factors specific to dosimeter type and period of use were applied and missing annual doses were estimated using a hierarchical nearby method to estimate deep dose equivalent for each worker. For early years with limited detection sensitivity, missed doses were quantified based on expected time-period-specific, low-dose statistical distributions. The revised dose estimates resulted in lower median and mean career doses than unadjusted data, while increasing the number of person-years with nonzero dose. Sensitivity analyses assessed the influence of bias in dosimetry measurements, missed doses and gap years on dose estimates. Differences in cumulative dose estimates between unadjusted and revised annual estimates are most prominent in the early operational years due to the highest bias during that time period.

dose reconstruction

Au-198 and TLD-600 results from IER-593 Godiva irradiations

This report summarizes the results from dosimetry packets deployed during a nominally 250 ◦C temperature rise Godiva IV burst. Dosimetry packets including Bare Au foils, Cd covered Au foils, and Thermoluminescent Dosimeters (TLDs) were deployed at five positions around Godiva at a height corresponding to the center height of the HEU fuel.

61 RADIATION PROTECTION AND DOSIMETRY

Logistics for the 2026 International Nuclear Accident Dosimetry Intercomparison Exercise

The purpose of this exercise is to test participants’ nuclear accident dosimeters (NADs) and personnel to the requirements established by American National Standards Institute (ANSI), Health Physics Society (HPS) standard ANSI/HPS-N13.3-2013 (R2025) Dosimetry for Criticality Accidents. IER-634 is the second nuclear accident dosimetry exercise taking place at the Armed Forces Radiobiology Research Institute (AFRRI) in Bethesda, MD, a Department of Defense (DOD) facility. This effort continues use of the high-dose neutron exposure test bed maintained by the DOD and represents the continued collaboration between the DOD and Department of Energy (DOE). Previous work at AFRRI included a reactor characterization (IER 484) in 2023 and a nuclear accident intercomparison exercise (IER-602) in 2024.

61 RADIATION PROTECTION AND DOSIMETRY

Predicting cutoff L-shells of solar protons using the GPPSn particle dataset

Solar energetic protons (SEPs) arriving at the Earth trigger severe radiation storms in the near-Earth space, directly impacting space missions operating at various altitudes. Therefore, monitoring SEP events and predicting the penetration depths of solar protons are critical for aerospace sectors. Building on previous efforts, here we demonstrate the feasibility of using proton measurements from the Global Prompt Proton Sensor network (GPPSn), enabled by Los Alamos National Laboratory developed combined X-ray dosimeters aboard GPS satellites, to characterize and predict the penetration of solar protons into the geomagnetic field. The inclined medium-Earth-orbits (MEOs) of the global GPS constellation offer a unique advantage of allowing simultaneous measurements of penetrating solar protons inside both open- and closed-field line regions. Therefore, the L-profiles of ∼10s–100 MeV solar protons and their associated cutoff L-shells can be determined from the GPPSn dataset, using predefined threshold proton flux values rather than traditional flux ratios. After examining a list of SEP event intervals across solar cycles 23, 24 and 25—including the 2024 Mother’s Day superstorm, we showcase how the latest GPPSn proton dataset (release v1.10), reprocessed and calibrated, can not only be used to monitor solar proton distributions inside the dynamic geomagnetic field for individual events, but also to derive a new empirical model linking cutoff L-shells with several key space weather parameters. This newly developed SEPCL-MEO model demonstrates high predictive performance; for example, predictions for > 30 MeV solar protons yield a correlation coefficient of 0.85 and performance efficiency of 0.67 when validated against GPPSn observations. Results from this pilot study underscores the scientific and operational value of the GPPSn dataset, and this dataset—when paired with machine-learning techniques—can play a critical role in observing and predicting the effects of future incoming SEP events, including extreme ones.

58 GEOSCIENCES