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Radon Photoionization: Project Technical Report

In most low-background physics experiments, radon is a significant and problematic source of background radiation because it is inert and sufficiently long-lived to pervade laboratory spaces. It may be possible to manipulate (and thus mitigate) radon electromagnetically by taking advantage of its relatively low first ionization energy. When considering ambient-temperature gas phases, only iodine is comparable. The other noble gases, and the most important constituents of breathable air (nitrogen and oxygen), all have higher ionization energies; so it may be possible to selectively manipulate radon in a variety of gas streams by ionizing it with an appropriately low-energy source of photons. Radon’s first ionization energy is in the vacuum UV part of the electromagnetic spectrum, which can be produced using a deuterium lamp. In this report, we present our attempts to manipulate radon via UV photoionization in a laboratory setting. This approach has the potential to increase radon removal efficiency from gases and/or to improve the efficiency of radon detectors. Unfortunately, our experiments suggest that either the life-time of a photoionized radon ion (before it re-neutralizes) is too short to be of much practical use and/or that our low-cost UV-photon source was not sufficiently energetic for efficient photoionization of radon.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A Review of Variables Impacting the Indoor Inhalation Radon Equilibrium Factor (FEQ)

With radon and its daughter products estimated as the second leading cause of lung cancer in the United States, it is imperative to understand their relative equilibrium inside commercial, community, and residential dwellings. The radon indoor inhalation fractional equilibrium factor (F eq ) quantifies the disequilibrium between radon and its progeny in indoor air, and recent advances have shown how air exchange rates (ACH) influence F eq . These numerically derived ACH-dependent F eq values are incorporated into the U.S. EPA's Radon Vapor Intrusion Screening Level (RVISL) calculator, which assists risk assessors in evaluating radon exposure. To advance the risk assessment science of actinon (Rn-219), thoron (Rn-220), and radon (Rn-222), the impact of variables such as indoor aerosol concentration and composition, outdoor air quality, household-specific characteristics, and environmental/meteorological conditions on the F eq must be examined. The primary objective of this research is to analyze these additional variables to determine the usefulness of incorporating such adjustment factors into the RVISL calculator and to identify areas of future research. Studies regarding the influence of these parameters are presented along with recommendations regarding the adjustment of the numerically derived F eq value. For example, elevated indoor aerosol concentrations, such as those originating from outdoor PM 2.5 or cigarette smoke, increase the abundance of accumulation- mode particles indoors, which in turn raises F eq values by facilitating the attachment of radon progeny to these aerosols. Smoking increases both the bronchial dose and F eq , while regions with high smog levels demonstrate the impact of regional air quality on F eq . In contrast, air cleaning systems and purifiers have been shown to reduce the F eq , suggesting that these systems could help mitigate radon exposure. Additionally, higher F eq values are typically observed during winter when ventilation rates are lower. This paper presents adjustment factors that may be applied to the RVISL F eq , emphasizing the need for further research to refine these variables and ensure accurate risk assessments in diverse environments. Applying these adjustment factors will minimize calculator over- and underestimations, providing a more accurate representation of the real-world risk associated with radon.

54 ENVIRONMENTAL SCIENCES↗

Using the Monte Carlo Method to Evaluate the Reliability of Screening Multifamily Housing for Radon

When screening for radon in a multifamily housing complex using a fixed sample density (e.g., testing 1 in 10 (10%) or 1 in 4 units (25%)), the statistical confidence is dependent upon the assumed elevated radon frequency. For example, testing 25% of units in a complex estimated to have eight units with elevated radon levels will provide 90% confidence. However, if it is assumed that, in the same complex, there are only three units with elevated radon levels, the confidence drops to around 58% for the same sample density. Furthermore, in the previous example, if elevated radon levels are not found during the screening, all that can be stated is that the screening provides 90% confidence that there are no more than seven units in the complex with elevated radon levels. To more fully illustrate this uncertainty, ten separate multifamily housing radon data sets with 1 to 10 units with radon levels ≥4 pCi/L (Table 1) were selected for analysis using the Monte Carlo statistical method. Unlike other mathematically based statistical approaches, the Monte Carlo statistical method relies on repeated analysis of randomly selected data. from a 100% sampled complex at various sample densities. Success for each simulation is defined as finding at least one unit with elevated radon levels. In this statistical method, confidence in the overarching conclusion can be greatly enhanced by repeating the simulated screening hundreds or even thousands of times. For this study, each of the ten data sets was simulated 1,000 times. For each simulation, the data set was randomized three times before the fixed percentage of data was selected.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Indoor Radon Measurements from Residential Buildings with Basements in a Community with Potential LLRW Contamination - 19566

The Port Hope Area Initiative (PHAI) represents the Government of Canada's commitment to the cleanup and safe, local, long-term management of historic low-level radioactive waste (LLRW) in two Southern Ontario municipalities-Port Hope and Clarington. The PHAI (see reference for internet address) is based on community-recommended solutions for the cleanup and safe long-term management of approximately 1.7 million cubic meters of LLRW. It is currently one of Canada's largest environmental remediation projects at a cost of over one billion dollars. Canadian Nuclear Laboratories (CNL) is implementing the PHAI on behalf of Atomic Energy of Canada Limited, a Federal Crown Corporation. An initial characterization and remediation program in the urban area of Port Hope was conducted from 1976 to 1981. The waste is the result of radium and uranium processing in Port Hope by the former Federal Crown Corporation Eldorado Nuclear Limited between 1933 and 1988. One contaminant of concern in the LLRW is radium-226 (Ra-226) which may lead to elevated indoor levels of radon-222 (Rn-222) indoors. As part of CNL's implementation of the PHAI, Arcadis is conducting the Port Hope Project Property Radiological Survey of approximately 4,800 small-scale sites to identify 1) properties that have not been affected by historic operations and 2) properties that have residual historic low-level radioactive waste impacts requiring remediation either for soils or for interior contamination or both. Over the last six years, a component of the Small Scale Sites (SSS) characterization surveys have measured radon concentrations in essentially all buildings in Port Hope using alpha-track detectors. All properties had subsurface characterization including analytical characterization and lithology following the radon measurement reporting to measure if soil concentrations exceeded the PHAI Cleanup Criteria (PHAI CC) for Ra-226 of 0.29 Bq/g. Buildings with radon gas exceeding a trigger level of 200 becquerels per cubic meter (Bq/m{sup 3}) or those with ventilation systems required investigation of soil concentrations around the perimeter of the building. Ra-226 concentrations above the background level of 0.05 Bq/g due to LLRW sources were forwarded to create remedial action plans (RAPs) to remove the contamination near the building. The SSS surveys provide a substantive data set on the approximately 3,000 properties measured to date with interior Rn-222 gas measurements and descriptions of the physical characteristics of the buildings, the lithology of soils near the buildings and the measurements of Ra-226 concentration in the soils on the property. Consideration of the potential for contribution from non-LLRW Ra-226 from natural sources or coal ash was required on some properties. This paper describes the data and exploratory analysis of the relationship(s) between LLRW and non-LLRW factors that affect the variation in indoor radon concentrations. Historical information on the urban area, the measured Ra-226 concentration and the age of the building were correlated with radon concentrations. A large variety of native soils are found in the complex terrain and the type of native soil was correlated with the radon concentrations. A statistical analysis to address the impact of co-related explanatory variables to model indoor radon concentrations is planned when the SSS activities are complete. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Study of radon concentration in wetland Mediterranean water using continuous monitoring - 25416

Radon is a radioactive gas that comes from the uranium and radium decay. It is considered the second cause of lung cancer in nonsmokers by the World Health Organization (WHO). Most studies focus on radon levels in air, which comes mainly from soil. Unfortunately, just some of them focus on radon in water which exposure is mainly due to radon inhalation when it is exhaled from water. In order to develop a methodology for radon measurement in water, this work compares two different techniques. The measurements have been done at Peniscola marsh, a location in the Valencian Community where significant radon concentrations have been measured in previous works. Furthermore, measurements in the Waste-Water-Treatment Plant (WWTP) near the marsh, where high radon concentrations have been found in air, are analyzed to confirm if they can be related to radon presence in water. (authors)

54 ENVIRONMENTAL SCIENCES↗

Characterization of Precipitation-Induced Radon Progeny Deposition Events Using a City-Scale Sensor Network

Networks of radiation detectors provide a platform for real-time radioactive source detection and identification in urban environments. Detection algorithms in these systems must adapt to naturally-occurring changes in background, which requires well-characterized relationships between precipitation events and their corresponding radiological signature. Here, we present a quantitative and qualitative description of rain-induced radon progeny deposition events occurring in Chicago from September 2023 to February 2024. We measure ambient gamma radiation levels, precipitation rate, temperature, pressure, and relative humidity in a network of sensor nodes. For each identified precipitation period, we decompose spectra into static- and radon-associated components as defined by a non-negative matrix factorization (NMF) algorithm. We find a consistent power-law relationship between a precipitation-dependent peak of the radon progeny proxy (RPP) and the peak strength of the radon-associated NMF component for most precipitation events. We conduct a case study of a rainfall period with abnormally high levels of implied radon progeny concentration and describe its temporal and spatial evolution. We hypothesize that this phenomenon is due to the air mass path that intersects a uranium-rich region of Wyoming. Finally, we cluster precipitation events into three distinct categories. One category roughly corresponds to events with deep low-pressure systems and high relative radon concentration, while another is characteristic of light stratiform rain with slightly higher temperatures and intermediate relative radon concentration. The third category appears to contain weak-gradient or lake breeze convection showers with intermittent precipitation and low relative radon concentration. These findings suggest that radiological anomaly detection could be improved by training unique background models corresponding to each category of meteorological event.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ultra-sensitive radon assay using an electrostatic chamber in a recirculating system

Rare event searches such as neutrinoless double beta decay and Weakly Interacting Massive Particle detection require ultra-low background detectors. Radon contamination is a significant challenge for these experiments, which employ highly sensitive radon assay techniques to identify and select low-emission materials. This work presents the development of ultra-sensitive electrostatic chamber (ESC) instruments designed to measure radon emanation in a recirculating gas loop, for future lower background experiments. Unlike traditional methods that separate emanation and detection steps, this system allows continuous radon transport and detection. This is made possible with a custom-built recirculation pump. A Python-based analysis framework, PyDAn, was developed to process and fit time-dependent radon decay data. Radon emanation rates are given for various materials measured with this instrument. A radon source of known activity provides an absolute calibration, enabling statistically-limited minimal detectable activities of 20 µBq. These devices are powerful tools for screening materials in the development of low-background particle physics experiments.

47 OTHER INSTRUMENTATION↗

Ultra-sensitive radon assay using an electrostatic chamber in a recirculating system

Rare event searches such as neutrinoless double beta decay and Weakly Interacting Massive Particle detection require ultra-low background detectors. Radon contamination is a significant challenge for these experiments, which employ highly sensitive radon assay techniques to identify and select low-emission materials. This work presents the development of ultra-sensitive electrostatic chamber (ESC) instruments designed to measure radon emanation in a recirculating gas loop, for future lower background experiments. Unlike traditional methods that separate emanation and detection steps, this system allows continuous radon transport and detection. This is made possible with a custom-built recirculation pump. A Python-based analysis framework, PyDAn, was developed to process and fit time-dependent radon decay data. Radon emanation rates are given for various materials measured with this instrument. A radon source of known activity provides an absolute calibration, enabling statistically-limited minimal detectable activities of 20 uBq. These devices are powerful tools for screening materials in the development of low-background particle physics experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radon Survey of Los Alamos National Laboratory Buildings and Los Alamos County Residential Buildings

A radon survey of office spaces was of interest to LANL for several reasons. First, exposure to natural radon in LANL office spaces has been considered to be outside the regulatory reach of the federal regulations and the U.S. Department of Energy (U.S. DOE) orders, and thus has not been studied as extensively as occupational exposure to other radionuclides and is not subject to the same rigorous radiological controls. Second, a general survey of radon concentrations in LANL workspaces was of interest to management to ensure safe environments for workers and is in keeping with the intent of OSHA requirements. Though radon in LANL offices would not be derived from enhanced radioactive sources, radon exposure in general office spaces has the potential to significantly impact worker risk. The purpose of the 2009 radon survey was to measure and document indoor radon levels across a broad spectrum of office-type workspaces and neighboring homes. The measured concentrations were compared against those measured across the United States and across the world. The results were also compared against a wide variety of radiation protection thresholds such as (1) the action levels of 148 Bq m -3 (the U.S. EPA action level for public housing), (2) ≈1,200 Bq m -3 OSHA threshold for office spaces, (3) effective dose threshold of 1 mSv threshold for defining a radiological worker, (4) 50 mSv occupational effective dose limit, and (5) 0.1 mSv and 1 mSv limits for public exposures from the air pathway and all pathways, respectively.

07 ISOTOPE AND RADIATION SOURCES↗

Low pressure radon diffusion - A laboratory study and its implications for lunar venting

Results of a study of radon migration through columns of fine particulate materials, at total pressures of 0.02-0.2 torr, are reported. Materials studied were: NBS Glass Spheres (SRM 1003), Emerson & Cuming Eccospheres (IG-101), activated coconut charcoal, Lipaci obsidian, and W-1 Standard Diabase. Rates of diffusion were used to derive heats of adsorption for radon on the materials tested. The most reliable values found clustered around 8-9 kcal/mole. These high heats of adsorption, if typical for most materials, combined with low percentages of radon emanation by lunar soils found by other researchers, imply that random walk diffusion will not be an important mechanism for redistributing the radon and the radon daughters produced in the lunar regolith. In particular, since random walk migration is not a sufficient mechanism to account for localized high concentrations of radon-222 and its daughter polonium-210 observed by the Apollo 15 and 16 command modules, an alternative mechanism is proposed, in which radon would be swept to the surface by other gases during intermittent venting events.

Friesen, L. J.↗

Radon-222 Charcoal Canister Steady State Model Calibrations Performed in a Highly Controlled Environmental Chamber and a Natural Indoor Environment

Charcoal canisters are a common method of 222 Rn screening. The calibrations of different batches of activated charcoal used in different canister designs are typically performed in large volume controlled environmental chambers with known and controlled radon concentration, temperature, and humidity. Radon screening could be facilitated in locations without ready access to environmental chambers if canisters could be accurately calibrated and undergo quality control in less controlled environments. This study compares charcoal canister calibrations from a highly controlled radon chamber with calibrations from a basement storage area experiencing temporally varying radon. In addition, the impacts of exposure time and spectral region of interest selection on calibration accuracy are investigated by comparing calibrations calculated using three different choices. Approximately 30 mo after calibrations were completed, groups of canisters were exposed for different durations of time to investigate measurement accuracy and calibration validity over an extended time. A digital simulation of charcoal canister kinetics was also performed to establish limits on how stable radon must be in a space for equilibrium-based calibration to be performed there. Overall, the accuracy of measurements using calibrations from each space differed by less than 10% after 2 d exposure time, showing that carefully controlled conditions are not necessary for the accurate calibration of charcoal canisters. Furthermore, measurement accuracy differed by less than 2% for different spectral region selections. Accuracy improved slightly with canister exposure duration. Simulations suggest that radon instability is most tolerable near the beginning of canister calibration exposures, but this merits further experimental study.

07 ISOTOPE AND RADIATION SOURCES↗

Radiological Characterization of Selected Thermal Centres Based on Indoor Radon Dosimetry - 17507

In countries with long historical tradition in thermal water therapy and with several mineral-medicinal thermal sources, workplaces within thermal centers may be a source of radon exposure which may be intensified if these are located in regions of high level of natural radiation. According to the EU Directive 96/29/Euratom (repealed by the Directive 2013/59/EURATOM) each Member State shall identify, by means of survey or any other adequate mean, the work activities where a significant increase in the exposure from natural radiation sources may occur, including thermal centers where the exposure to thoron/radon daughters or gamma radiation may occur. The purpose of this work was to perform a radiological characterization of selected thermal centers based on indoor dosimetry. The effective doses received by workers due to radon inhalation were estimated and gamma dose rates were measured through continuous periods. The radon risk for indoor exposure was assessed on a probabilistic basis both on thermal centers and workers' dwellings. Radon levels within the thermal centers ranged from 73 to 4335 Bq/m{sup 3} and the values within the workers dwellings are of the same order of magnitude, 68-4051 Bq/m{sup 3}. Approximately 66 % of indoor radon concentration values are above the maximum EU reference (300 Bq/m{sup 3}) and 94 % of the effective dose is higher than 1 mSv/year. In some situations, radon levels at residential environments are much higher than at workplaces and effective doses are higher than 6 mSv/year, both at residential and work environments. (authors)

61 RADIATION PROTECTION AND DOSIMETRY↗

Challenges and Practical Solutions for Conducting Structural MARSSIM Surveys in Elevated Radon Environments - 20413

The Multi-Agency Radiation Survey and Site Investigation Manual (MARSSIM) [1] provides comprehensive guidance for the development and implementation of radiological surveys conducted to demonstrate compliance with a dose- or risk-based cleanup goal during final status survey. The MARSSIM methodology follows an integrated strategy combining direct measurements and sampling to assess uniform residual contamination, and scanning surveys to identify localized areas of elevated activity. Building surveys assessing residual surface contamination present unique challenges from reliance on field measurements that may be subject to less than ideal environmental conditions. Additionally, limited characterization and excessive conservatism incorporated into the conceptual site model may result in derived concentration guideline levels (DCGL) and, as a consequence of relatively inefficient field instrumentation, corresponding attributable count rates generally comparable to background. The presence of elevated ambient radon concentrations and associated progeny deposition both exacerbate these intrinsic survey challenges and introduce a series of technical, logistic, and administrative obstacles that can wreak havoc on the statistical legitimacy of each component of the MARSSIM process. Short-lived radon progeny including polonium-218, lead-214, bismuth-214, and polonium-214 produce excessive alpha and beta radiation that may decrease instrument sensitivity through an increase in background count rates, and, at worst, may result in incorrect survey unit failure through the simulation of residual surface activity. Aside from the obvious solution of exhaustive radon mitigation, the primary objectives are to distinguish between radon progeny deposition and actual surface activity, and collect sufficient defensible data. The following is a technical discussion of the consequences of performing building MARSSIM surveys in the presence of elevated ambient radon atmospheres, conceptual examples, and an overview of practical strategies to minimize the effects of radon interference while collecting sufficient defensible data to complete the survey. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radon 222 tracing of soil and forest canopy trace gas exchange in an open canopy boreal forest

A set of continuous, high-resolution atmospheric radon (Rn-222) concentration time series and radon soil flux measurements were acquired during the summer of 1990 at a micrometeorological tower site 13 km northwest of Schefferville, Quebec, Canada. The tower was located in a dry upland, open-canopy lichen-spruce woodland. For the period July 23 to August 1, 1990, the mean radon soil flux was 41.1 +/- 4.8 Bq m(exp -2)/h. Radon surface flux from the two end-member forest floor cover types (lichen mat and bare soil) were 38.8 +/- 5.1 and 61.8 +/- 15.6 Bq m(exp -2)/h, respectively. Average total forest canopy resistances computed using a simple 'flux box' model for radon exchange between the forest canopy and the overlying atmosphere range from 0.47 +/- 0.24 s cm(exp -1) to 2.65 +/- 1.61 cm(exp -1) for daytime hours (0900-1700 LT) and from 3.44 +/- 0.91 s cm(exp -1) to 10.55 +/- 7.16 s cm(exp -1) for nighttime hours (2000-0600) for the period July 23 to August 6, 1990. Continuous radon profiling of canopy atmospheres is a suitable approach for determining rates of biosphere/atmosphere trace gas exchange for remote field sites where daily equipment maintenance is not possible. where daily equipment maintenance is not possible.

Ussler, William, III↗

US EPA Superfund Radon Vapor Intrusion Screening Level (RVISL) Electronic Calculator - 20340

Currently, there is no U.S. Environmental Protection Agency (EPA) guidance on correlating soil or groundwater levels of radon with indoor radon concentrations at Superfund sites. EPA is developing the Radon Vapor Intrusion Level Calculator (RVISL) Calculator which is an online tool. The RVISL calculator: (1) lists three radon isotopes (Rn-219, Rn-220 and Rn-222) known to pose a potential cancer risk through the inhalation pathway; (2) provides generally recommended risk and Applicable or Relevant and Appropriate Requirements (ARAR) based preliminary remediation goals (PRG) for groundwater, soil gas (exterior to buildings and sub-slab) and indoor air for default target risk and ARAR based levels and exposure scenarios; and (3) allows calculation of site-specific PRGs based on user-defined target risk and ARAR based levels and exposure scenarios. EPA developed the RVISL calculator to help risk assessors, remedial project managers, and others involved with risk assessment and decision making at radioactively contaminated sites. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Delegated Regressor, A Robust Approach for Automated Anomaly Detection in the Soil Radon Time Series Data

We propose a new method based on the idea of delegating regressors for predicting the soil radon gas concentration (SRGC) and anomalies in radon or any other time series data. The proposed method is compared to different traditional boosting e.g., Extreme Gradient Boosting (EGB) and simple regression methods e.g., support vector regressors with linear kernel and radial kernel in terms of accurate predictions. R language has been used for the statistical analysis of radon time series (RTS) data. The results obtained show that the proposed methodology predicts SRGC more accurately when compared to different traditional boosting and regression methods. The best correlation is found between the actual and predicted radon concentration for window size of 2 i.e., two days before and after the start of seismic activities. RTS data was collected from 05 February 2017 to 16 February 2018, including 7 seismic events recorded during the study period. Findings of study show that the proposed methodology predicts the SRGC with more precision, for all the window sizes, by overlapping predicted with the actual radon time series concentrations.

54 ENVIRONMENTAL SCIENCES↗

An age- and sex-specific biokinetic model for radon *

Publication 137 of the International Commission on Radiological Protection (ICRP) describes a biokinetic model for radon used to derive dose coefficients for occupational intake of radon isotopes. The model depicts transfer of inhaled or ingested radon to blood, exchange of radon between blood and tissues, and gradual loss of radon from the body based on physical laws governing transfer of a non-reactive and soluble gas between materials. Here, this paper describes an age- and sex-specific variation of that model developed for use in an upcoming ICRP series of reports on environmental intake of radionuclides by members of the public titled ‘Dose Coefficients for Intakes of Radionuclides by Members of the Public’. The proposed model modifies the model structure and transfer coefficients presented in Publication 137 to allow more realistic dosimetric treatment of bone marrow and breast and expands the model to address pre-adult ages, based on the physical principles used in the development of the model of Publication 137 together with anatomical and physiological changes occurring during human development.

61 RADIATION PROTECTION AND DOSIMETRY↗

Two-stage model of radon-induced malignant lung tumors in rats: effects of cell killing

A two-stage stochastic model of carcinogenesis is used to analyze lung tumor incidence in 3750 rats exposed to varying regimens of radon carried on a constant-concentration uranium ore dust aerosol. New to this analysis is the parameterization of the model such that cell killing by the alpha particles could be included. The model contains parameters characterizing the rate of the first mutation, the net proliferation rate of initiated cells, the ratio of the rates of cell loss (cell killing plus differentiation) and cell division, and the lag time between the appearance of the first malignant cell and the tumor. Data analysis was by standard maximum likelihood estimation techniques. Results indicate that the rate of the first mutation is dependent on radon and consistent with in vitro rates measured experimentally, and that the rate of the second mutation is not dependent on radon. An initial sharp rise in the net proliferation rate of initiated cell was found with increasing exposure rate (denoted model I), which leads to an unrealistically high cell-killing coefficient. A second model (model II) was studied, in which the initial rise was attributed to promotion via a step function, implying that it is due not to radon but to the uranium ore dust. This model resulted in values for the cell-killing coefficient consistent with those found for in vitro cells. An "inverse dose-rate" effect is seen, i.e. an increase in the lifetime probability of tumor with a decrease in exposure rate. This is attributed in large part to promotion of intermediate lesions. Since model II is preferable on biological grounds (it yields a plausible cell-killing coefficient), such as uranium ore dust. This analysis presents evidence that a two-stage model describes the data adequately and generates hypotheses regarding the mechanism of radon-induced carcinogenesis.

NASA Program Radiation Health↗