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Simulation of radon-222 with the GEOS-Chem global model: Emissions, seasonality, and convective transport

Radon-222 (222Rn) is a short-lived radioactive gas naturally emitted from land surface, and has long been used to assess convective transport in atmospheric models. In this study, we simulate 222Rn using the GEOS-Chem chemical transport model with aims to improve our understanding of 222Rn emissions and surface concentration seasonality, and to characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, MERRA and GEOS-FP. We evaluate four available 222Rn emission scenarios by comparing model results with surface observations at 51 global surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with global surface observations (< 70% data within a factor of 2) and a large underestimate of wintertime surface 222Rn concentrations at Northern Hemisphere mid- and high-latitudes due to an oversimplified formulation of 222Rn emission fluxes (1 atom cm-2 s-1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global 222Rn emission scenario based on Zhang et al. (2011) and show its potential to improve simulated surface 222Rn concentrations and seasonality. The regional components of this emission scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors to 222Rn emission flux rates. However, large model underestimates of surface 222Rn concentrations still exist in Asia, suggesting unusually high regional 222Rn emissions. We propose a conservative up-scaling factor of 1.2 for 222Rn emission fluxes in China, as also constrained by the observed deposition fluxes of 210Pb (decay daughter of 222Rn). With this modification, the model shows better agreement with the observations in Europe and North America (>80% data within a factor of 2), and reasonable agreement in Asia (close to 70%). Further constraints on 222Rn emissions would require additional observations of surface 222Rn concentrations and emission fluxes in central U.S., Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed 222Rn vertical profiles during northern mid-latitude summertime and from two short-term airborne campaigns. While the simulations with both GEOS products are able to capture the observed vertical gradient of 222Rn concentrations in the lower troposphere (0-4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared to GEOS-FP, MERRA leads to stronger convective transport of 222Rn, which is partially compensated by its weaker large-scale vertical advection, resulting in similar global vertical distributions of 222Rn concentrations between the two simulations.

Zhang, Bo↗

Simulation of Radon-222 with the GEOS-Chem Global Model: Emissions, Seasonality, and Convective Transport

Radon-222 (Rn-222) is a short-lived radioactive gas naturally emitted from land surfaces and has long been used to assess convective transport in atmospheric models. In this study, we simulate Rn-222 using the GEOS-Chem chemical transport model to improve our understanding of Rn-222 emissions and surface concentration seasonality and characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, the Modern-Era Retrospective analysis for Research and Applications (MERRA) and GEOS Forward Processing (GEOS-FP). We evaluate four global Rn-222 emission scenarios by comparing model results with observations at 51 surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with surface observations globally (68.9 % of data within a factor of 2) and a large underestimate of winter surface Rn-222 concentrations at Northern Hemisphere midlatitudes and high latitudes due to an oversimplified formulation of Rn-222 emission fluxes (1 atom cm−2 s−1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global Rn-222 emission scenario based on Zhang et al. (2011) and demonstrate its potential to improve simulated surface Rn-222 concentrations and seasonality. The regional components of this scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors in determining Rn-222 emission flux rates. However, large model underestimates of surface Rn-222 concentrations still exist in Asia, suggesting unusually high regional Rn-222 emissions. We therefore propose a conservative upscaling factor of 1.2 for Rn-222 emission fluxes in China, which was also constrained by observed deposition fluxes of 210Pb (a progeny of Rn-222). With this modification, the model shows better agreement with observations in Europe and North America (> 80 % of data within a factor of 2) and reasonable agreement in Asia (close to 70 %). Further constraints on Rn-222 emissions would require additional concentration and emission flux observations in the central United States, Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed Rn-222 vertical profiles in northern midlatitude summer and from three short-term airborne campaigns. While simulations with both GEOS products are able to capture the observed vertical gradient of Rn-222 concentrations in the lower troposphere (0–4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared with GEOS-FP, MERRA leads to stronger convective transport of Rn-222, which is partially compensated for by its weaker large-scale vertical advection, resulting in similar global vertical distributions of Rn-222 concentrations between the two simulations. This has important implications for using chemical transport models to interpret the transport of other trace species when these GEOS products are used as driving meteorology.

Bo Zhang↗

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↗

Radon-222 in the lunar atmosphere.

In 1969 Yeh and Van Allen set upper limits for the alpha-particle emissivity of the moon. The equilibrium surface activity reported by Turkevich et al. (1970) for each alpha active Rn-222 daughter at Mare Tranquillitatis cannot be reconciled with existing diffusion theory. The data, therefore, suggest that earth based diffusion constants are not applicable in the vacuum conditions of the moon, or that there are substantial variations in the uranium content of the moon over relatively small distances.

Brodzinski, R. L.↗

Radon-222 as a test of convective transport in a general circulation model

A three-dimensional tracer model based on the Goddard Institude of Space Studies GCM is used to simulate the distribution of Rn-222 over North America to test the ability of the model to describe the transport of pollutants in the boundary layer and the exchange of mass between the boundary layer and the free troposphere. The model results are compared with surface observations from five sites in the U.S., showing that Rn-222 concentrations are primarily regulated by dry convection. The simulations show satisfactory agreement with observations although the model underpredicts observations at night and the simulated Rn-222 concentrations over the northeastern U.S. are too high in the spring and too low in the fall.

Jacob, Daniel J.↗

A global numerical study of radon-222 and lead-210 in the atmosphere using the AES and York University CDT General Circulation Model (AYCG)

The Canadian Climate Center (CCC) GCM has been modified to allow its use for studies in atmospheric chemistry. The initial experiments reported here have been run to test and allow sensitivity studies of the new transport module. The impact of different types of parameterization for the convective mixing have been studied based on the large scale evolution of Rn-222 and Pb-210. Preliminary results have shown that the use of a scheme, which mixes unstable columns over a very short time scale, produces a global distribution of lead that agrees in some aspects with observations. The local impact of different mixing schemes on a short lived tracer like the radon is very important.

Beagley, Stephen R.↗

Rn-222 tracing and stable isotope measurements of biogenic gas fluxes from methane saturated sediments

Transport of reduced biogenic gases from anoxic sediments and soils to the atmosphere can be quantitatively studied through measurement of radon-222/radium-226 disequilibrium. In previous work, seasonal variations in biogenic gas transport mechanisms, net fluxes and overall composition were documented. Now presented are direct field measurements of radon-222 activity in gases exiting organic rich sediments which show their usefulness for tracing of the stripping of dissolved biogenic gases from within the sediment column and transport via bubble ebullition. Methane is depleted in deuterium during the summer as compared with winter months and is in general lighter than in most marine sediments signaling the probable importance of acetate as an important precursor molecule. The significant seasonal isotopic variations observed illustrate the importance of understanding mechanisms and rates of biogenic gas production in order to interpret observed tropospheric isotopic data.

Martens, Christopher S.↗

Riverbed and Near-Surface Water Quality Data, Hanford Reach, Columbia River, February 2021 - April 2022

This dataset contains longitudinal profiles of natural groundwater tracers (temperature, electrical conductivity (EC), and Radon-222 (Rn)) collected to identify locations of hydrologic exchange flows along a 75-km reach of the Columbia River near Richland, Washington.A jetboat was used to tow a 30 foot long, weighted tether that had one set of temperature and EC sensors just below the water surface and one set of temperature and EC sensors on the end (just above the river bed). The dataset contains profiles of temperature/EC data (resolution: 1 second) collected along the left and right banks during three different sampling events. During the final sampling event, we revisited some "deep holes" where the river was more than 30 feet deep with a weighted tether that was 75 feet long. The dataset has been processed to remove data collected when the sensors were not in the water, or when the water was too deep to keep the tether on the riverbed. We collected grab samples of water for analysis of dissolved Rn in places where the temperature/EC was different from the background river water. The Rn data was joined to the temperature/EC profiles based on the sample times.This dataset is comprised of one main data folder containing (1) file-level metadata; (2) data dictionary; (3) installation methods; (4) February 2021 data; (5) July 2021 data; (6) April 2022 data; and (7) April 2022 deep hole data. All files are .csv format and can be opened with a spreadsheet program (such as Microsoft Excel or OpenOffice).

54 ENVIRONMENTAL SCIENCES↗

System Model Calculations for the Active Trenches of the Low-Level Burial Grounds, Hanford Site, Washington

Two lined trenches (Trench 31 and 34) located within the 200 West Low-Level Burial Ground (LLBG) area of the U.S. Department of Energy’s (DOE) Hanford Site are designated for permanent disposal of low-level radioactive waste (LLW) and mixed low-level radioactive waste (MLLW). In accordance with DOE O 435.1, Radioactive Waste Management, radioactive waste shall be managed and disposed in a manner that is protective of worker, public health and safety, and the environment. DOE O 435.1 requires a site-specific radiological performance assessment (PA) that includes calculations of potential releases and subsequent doses to members of the public for a period of 1,000 years after closure of a low-level waste (LLW) disposal facility. The purpose of this environmental calculation file (ECF) is to document the various dose calculations performed to support DOE’s LLBG PA. The dose assessments are performed to evaluate the potential exposure of an all-pathway representative person to radionuclide contaminants of potential concern (COPCs) that may be released from the LLBG Trenches 31 and 34 to the point of calculation (POC) located at the outer edge of a 100 m buffer zone surrounding the trench boundary. This ECF uses inputs from other ECFs and their associated model package reports (MPRs) supporting the LLBG PA. The five major objectives of this ECF are to present the results of the following: (1) Deterministic dose assessments for both groundwater and atmospheric exposure scenarios; (2) Radon-222 (Rn-222) flux emanating at the surface from the disposed wastes; (3) Uncertainty analyses of the groundwater pathway annual dose due to uncertainty in input parameters; (4) Sensitivity analyses of the input parameters that could potentially impact the fate and transport of the contaminants and doses; (5) Doses arising from inadvertent intruder exposure scenarios.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Detection of radon emission at the edges of lunar maria with the Apollo alpha-particle spectrometer

The distribution of radioactive polonium-210, a decay product of radon-222, shows enhanced concentrations at the edges of lunar maria. Enhancements are seen at the edges of Mare Fecunditatis, Mare Crisium, Mare Smythii, Mare Tranquillitatis, Mare Nubium, Mare Cognitum, and Oceanus Procellarum. The observation is indicative of the transient emission of radon gas from the perimeters of lunar maria.

Gorenstein, P.↗

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.↗

Recent activity in the moon; Proceedings of the Special Symposium, Houston, Tex., March 16, 1976

The papers review evidence for recent activity within the moon as manifested by lunar grid system, transient phenomena, moonquakes, and episodic emissions of radiogenic gases. Topics include a survey of lunar transient phenomena, possible causes of such phenomena, evidence that high-frequency seismic events may be shallow moonquakes, lunar seismicity and tectonics, a hypothesis on the nature of sites of lunar gas venting, and a search for sporadic gas emissions from the moon. Other contributions discuss the release of radiogenic argon-40 from the moon, radon-222 emission as an indicator of current activity on the moon, upper limits to gas emission from sites of lunar transient phenomena, physical processes that could produce transient changes on the lunar surface, critical-velocity gas-plasma interaction as a mechanism for lunar transient phenomena, and tidal triggering of moonquakes, transient phenomena, and radiogenic-gas emissions.

Runcorn, S. K.↗

Gaseous constituents in the plume from eruptions of Mount St. Helens

Measurements in the stratosphere of gaseous constituents in the plume of Mount St. Helens were obtained during five flights of the NASA U-2 aircraft between 19 May and 17 June 1980. Mixing ratios from gas chromatographic measurements on samples acquired about 24 hours after the initial eruption show considerable enhancement over nonvolcanic concentrations for sulfur dioxide (more than 1000 times), methyl chloride (about 10 times), and carbon disulfide (more than 3 times). The mixing ratio of carbonyl sulfide was comparable to nonvolcanic mixing ratios although 3 days later it was enhanced two to three times. Ion chromatography measurements on water-soluble constituents are also reported. Very large concentrations of chloride, nitrate, and sulfate ions were measured, implying large mixing ratios for the water-soluble gaseous constituents from which the anions are derived. Measurements of radon-222 present in the plume are also reported.

Inn, E. C. Y.↗

The effect of wind and currents on gas exchange in an estuarine system

The objectives were to develop a non-volatile tracer to use in gas exchange experiments in laterally unconfined systems and to study applications of deliberate tracers in limnology and oceanography. Progress was made on both fronts but work on the development of the non-volatile tracer proved to be more difficult and labor intensive that anticipated so no field experiments using non-volatile tracers was performed as yet. In the search for a suitable non-volatile tracer for an ocean scale gas exchange experiment a tracer was discovered which does not have the required sensitivity for a large scale experiment, but is very easy to analyze and will be well suited for smaller experiments such as gas exchange determinations on rivers and streams. Sulfur hexafluoride, SF6, was used successfully as a volatile tracer along with tritium as a non-volatile tracer to study gas exchange rates from a primary stream. This is the first gas exchange experiment in which gas exchange rates were determined on a head water stream where significant groundwater input occurs along the reach. In conjunction with SF6, Radon-222 measurements were performed on the groundwater and in the stream. The feasibility of using a combination of SF6 and radon is being studied to determine groundwater inputs and gas exchange of rates in streams with significant groundwater input without using a non-volatile tracer.

Broecker, W. S.↗

Evolving radon diffusion through earthen barriers at uranium waste disposal sites

Field measurements of Rn-222 fluxes from the tops and bottoms of compacted clay radon barriers were used to calculate effective Rn diffusion coefficients (D Rn ) at four uranium waste disposal sites in the western United States to assess cover performance after more than 20 years of service. Values of D Rn ranged from 7.4 × 10 -7 to 6.0 × 10 -9 m 2 /s, averaging 1.42 × 10 -7 . Water saturation (S W ) from soil cores indicated that there was relatively little control of D Rn by S W , especially at higher moisture levels, in contrast to estimates from most steady-state diffusion models. Further, this is attributed to preferential pathways intrinsic to construction of the barriers or to natural process that have developed over time including desiccation cracks, root channels, and insect burrows in the engineered earthen barriers. A modification to some models in which fast and slow pathway D Rn values are partitioned appears to give a good representation of the data; 4% of the fast pathway was needed to fit the data regression. For locations with high S w and highest D Rn (and fluxes) at each site, the proportion of fast pathway ranged from 1.7% to 34%, but for many locations with lower fluxes, little if any fast pathway was needed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗