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Application of Nuclear Technology to Art Identification Problems: First Annual Report

Throughout the centuries, as man has become increasingly affluent, his interest in antiquities and objects of art, and the price he has been willing to pay for them, has increased. Inevitably, one result has been to attract the unscrupulous to the production and sale of counterfeit paintings, sculptures, and other works of art. The skill of forgers varies but often is highly sophisticated. However, dealers, museum curators, and other experts have also become more skillful in the detection of forgeries. Scientific tools of increasing sensitivity and sophistication have gradually been applied to the examination of the materials of art and archaeology. Such tools frequently support and render more reliable the judgment of the experts. The quality of forgeries may improve further as their makers become acquainted with the new methods of detection and in turn learn to circumvent or confound the methods. Therefore, the development of still more advanced methods of examination has great utility in the art world. This is particularly true if the ultimate effect is to make circumvention of the methods of examination so costly that the economic incentives for producing forgeries may be substantially reduced, if not eliminated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Removal of {sup 222}Rn daughters from metal surfaces

Removal of the long-lived {sup 222}Rn daughters ({sup 210}Pb, {sup 210}Bi and {sup 210}Po) from copper, stainless steel and germanium surfaces was investigated. As cleaning techniques etching and electro-polishing was applied to samples in a form of discs exposed earlier to a strong radon source. Reduction of the {sup 210}Pb activity was tested using a HPGe spectrometer, for {sup 210}Bi a beta spectrometer and for {sup 210}Po an alpha spectrometer was used. According to the conducted measurements electro-polishing was always more efficient compared to etching and in case of copper the activity reduction factors for {sup 210}Pb, {sup 210}Bi and {sup 210}Po were between 200 and 400. Etching does not remove {sup 210}Po from copper but works very efficiently from germanium. Results obtained for {sup 210}Pb and {sup 210}Bi for etched stainless steel were worse but still slightly better than those achieved for copper.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

SU-F-P-24: Radiological Disperse Device

Purpose: We are now living in a society of constant fear of terrorism. This topic is pertaining to give a general knowledge of what is a radiological dispersion device or RDD and in case of its detonation, what are the options open to public for a safe action in terms of reducing the exposure and knowing the proper steps. These RDD are also called dirty bombs. Methods: Compared to nuclear weapons, dirty bombs are easy to make. In order for a terrorist organization to construct and detonate a dirty bomb, it must acquire radioactive material by stealing it or buying it through legal or illegal channels. Possible RDD material could come from the millions of radioactive sources used in the industry, for medical purposes and in academic applications mainly for researches. These are, americium-{sup 241}, californium-{sup 252}, caesium-{sup 137}, cobalt-{sup 60}, iridium-{sup 192}, plutonium-{sup 238}, polonium-{sup 210}, radium-{sup 226} and strontium-{sup 90}. Results: Prompt detection of the type of radioactive material used will greatly assist advising people on the protective measures, like sheltering in place, or quickly leaving the immediate area. The effects of radiation are determined by:°the amount of radiation absorbed by body°the type of radiation °the distance from the radiation to an individual°the means of exposure absorbed by the skin, inhaled, or ingested; and length of time exposed. Conclusion: In any facility it is now much more important to keep a log list of all radioactive materials in use. In case there is a dirty bomb explosion, the chaos and economic cost could be enormous. The economic cost for the evaluation of the contamination, survey of people and surroundings and the after treatment, decontamination cost and effort will be a big challenge in any country. So awareness and preparation is the start to face this new type of challenge.

61 RADIATION PROTECTION AND DOSIMETRY↗

Comparison of {sup 238}U, {sup 210}Po and {sup 210}Pb Speciation in Six Different Types of Soils

Speciation of {sup 238}U, {sup 210}Po and {sup 210}Pb in six different types of Syrian soil (Entisols, Inceptisol, Aridisol, Mollisols, Vertisols and Rock outcrops) was studied using a four-step sequential extraction procedure. The binding nature of {sup 238}U, {sup 210}Po and {sup 210}Pb was correlated with soil properties including soil particles, pH, EC, OM, sand, silt and clay. The results showed that the exchangeable and carbonate fractions of {sup 238}U did not exceed 10%. In addition, the {sup 238}U, {sup 210}Po and {sup 210}Pb fractions bonded to organic matter increased as the soil clay content decreased. The highest {sup 210}Po fraction was found to be bonded to soil Fe/Al/Mn-oxides for Entisols soils (56%) and silica for Aridisol soils (53%). Soil clay content showed a linear correlation with {sup 210}Po concentrations in soils ranging from 0.34 to 0.91. The results are considered useful in assessing the risks resulting from soils contaminated by naturally occurring radioactive material from the phosphate and oil industry.

07 ISOTOPE AND RADIATION SOURCES↗

Nuclear Data Sheets for A = 210

Evaluated spectroscopic data for {sup 210}Au, {sup 210}Hg, {sup 210}Tl, {sup 210}Pb, {sup 210}Bi, {sup 210}Po, {sup 210}At, {sup 210}Rn, {sup 210}Fr, {sup 210}Ra, {sup 210}Ac, and {sup 210}Th and corresponding level schemes from radioactive decay and reaction studies are presented. This evaluation supersedes the previous evaluation by E. Browne (2003Br13). Highlights of this publication are the identification of new μs isomers of {sup 210}Hg by 2013Go10 and measurement of an excited level energy at 1709 keV 30 of {sup 210}Rn from {sup 214}Rn α decay: 68.6 μs by 2006Ku26 denoted as x+1664.6 in the Adopted Levels. Earlier experimental limits for x≤50 keV was proposed in 1979Po19 and 1982Po03 – (HI,xnγ)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Modeling of Lead-210 Data Documents Benefits in Proactively Understanding TENORM Deposition - 18515

Radioactive decay of naturally occurring Radon-222 present in just-produced natural gas can lead to deposition of its radiogenic daughter, Lead-210, and subsequent radiogenic progeny within natural gas handling, treatment, and distribution facilities. Worker safety issues and disposal challenges arise when these accumulate to radiologically problematic activity levels. This is due to the 22.3-year half-life of Lead-210, allowing for multi-decade period of accumulation to occur and to persist, even after facility operations have ceased. Due to the far shorter half-lives of Lead-210 radiogenic progeny, especially that of Polonium-210, secular equilibrium within the Lead-210-Bismuth-210-Polonium-210 decay chain is quickly approached during facility operations and achieved after facility operations end. Lead-210 that accumulates in pipe scale can complicate any subsequent intrusive facility modifications, such as disassembly and dismantlement, potentially exposing workers to adverse radioactivity and impeding recycling and/or disposal of radiologically impacted equipment or other material. Experience has shown it is not strictly the presence of Lead-210 that is problematic but rather its 'unexpected' presence when this Technologically Enhanced Naturally Occurring Radioactive Material (TENORM) is discovered during intrusive work not incorporating radiological health and safety and material handling plans. Conversely, when implementing a program that proactively considers the potential for Lead-210, this form of TENORM simply becomes another 'special waste' that can be safely, efficiently, and effectively addressed during a decommissioning effort, without associated adverse worker exposures, project cost over-runs, and schedule delays. This paper will discuss how proactive radioactive scanning quickly and safely identified Lead-210 and its radiogenic progeny within a natural gas sweetening and compressor station located in northern Montana, a portion of which was undergoing decommissioning, aiding in safe and compliant material handling and recycling. The location of this operation necessitated that the decommissioning program be completed on schedule to prevent weather-related impacts due to the onset of adverse winter conditions. Further, the radioactive data acquired during this project will be shown to provide important insight into historic behavior of Lead-210 in terms of its disposition and its more recent decay. From these data, it became possible to back-model the average activity of Radon-222 within the natural gas being processed during the life of the operation, how the estimated Radon-222 activity within the processed natural gas conformed to measured Radon-222 at various other natural gas fields, and how this information can be leveraged in developing safe and successful plans for future intrusive work at this and companion site operations. This presentation will also note the apparent preferential accumulation of Lead-210 within both rubber-based materials, such as gaskets and seals, and grease-based products found within natural gas flow lines. Thoughts regarding processes that may lead to this finding will be explored. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Uptake behavior of 73 As, 75 Se, 197m Hg, 212 Pb and 210 Po on Eichrom pre-filter resin from HCl and HNO 3

We report the extraction of 73 As, 75 Se, 197 mHg, 212 Pb and 210 Po on Eichrom pre-filter resin was studied in HCl and HNO 3 with batch uptake, kinetic and column experiments. There was significant extraction of mercury in HNO 3 and HCl, and polonium and selenium in HCl. The kinetics are sufficient to allow for retention on pre-filter columns, and separations of 73 As from 75 Se and 197 mHg, and 212 Pb from 210 Po are demonstrated. This retention is important for the development of chemical separations as pre-filter resin is commonly used alongside extraction chromatography resins but its potential for uptake of metal ions is not well characterized.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

The polonium-210 poisoning of Mr Alexander Litvinenko

Mr Litvinenko died on 23rd November 2006 after having been poisoned with polonium-210 on 1st November. Measurements of the polonium-210 content of post-mortem tissue samples and samples of urine and blood showed the presence of large amounts of 210 Po. Furthermore, autoradiography of hair samples showed two regions of 210Po activity, providing evidence of an earlier poisoning attempt during October 2006, resulting in absorption to blood of about one-hundredth of that estimated for 1st November. Intake by ingestion on 1st November was estimated to be around 4 GBq, assuming 10% absorption to blood, and the resulting organ doses reached estimated values that were generally in a range from about 20 Gy to over 100 Gy. In comparison with estimates of protracted alpha particle the doses required to cause irreversible organ damage support the conclusion that death was the inevitable consequence of multiple organ failure, with destruction of the haemopoietic bone marrow, as well as damage to kidneys and liver, being important contributors. If the earlier poisoning during October 2006 had not been followed by a second major intake on 1st November, it is possible that the earlier intake of around 40 MBq, with absorption of 4 MBq to blood, might have proved fatal over a prolonged period of months or years, primarily as a result of kidney damage following a dose of approaching 3 Gy.

61 RADIATION PROTECTION AND DOSIMETRY↗

Evaluation and mitigation of trace 210Pb contamination on copper surfaces

Clean materials are required to construct and operate many low-background physics experiments. High-purity copper has found broad use because of its physical properties and availability. In this paper, we describe methods to assay and mitigate Pb-210 contamination on copper surfaces, such as from exposure to environmental radon or coming from bulk impurities. We evaluated the efficacy of wet etching on commercial samples and observed that Po-210 contamination from the copper bulk does not readily pass into solution. During the etch, the polonium appears to trap at the copper-etchant boundary, such that it is effectively concentrated at the copper surface. We observed a different behavior for Pb-210; high-sensitivity measurements of the alpha emissivity versus time indicate the lowest level of Pb-210 contamination ever reported for a commercial copper surface: 0 +/- 12 nBq/cm2 (1-sigma). Additionally, we have demonstrated the effectiveness of mitigating trace Pb-210 and Po-210 surface backgrounds using custom, high-purity electroplating techniques. These approaches were evaluated utilizing assays performed with an XIA UltraLo-1800 alpha spectrometer.

radon, copper, copper cleaning, dark matter, Pb-21↗

Novel rapid oxidizing fusion method to determine Polonium-210 in air filters

A rapid method for the determination of polonium-210 in air filters has been created for use following a radiological event and for routine environmental monitoring. Air filter samples, including cellulose and glass fiber, are fused with a sodium or potassium nitrate/sodium hydroxide flux material. The alkaline matrix minimizes polonium volatility during sample digestion steps, while efficiently dissolving the air filter and inorganic matter implanted on the filter. The addition of nitrate to the flux destroys organic material which can decrease Polonium recovery during precipitation, extraction and source preparation steps. Polonium is concentrated and separated from the sample matrix using an iron hydroxide precipitation and extraction chromatography with DGA Resin. Polonium-210 is subsequently measured by alpha spectrometry following rapid microprecipitation with bismuth phosphate. The new method employs extraction chromatographic purification to remove alpha emitting interferences and sample matrix constituents which can interfere with 210 Po measurements using alpha spectrometry. The novel blend of sodium hydroxide and alkali metal nitrate digests the air filters quickly and effectively.

61 RADIATION PROTECTION AND DOSIMETRY↗

Environmental evaluation of radioactivity levels and associated radiation hazards in groundwater around the WIPP site

Groundwater may contain radioactive substances which can be dangerous to human health. Concentrations of natural radionuclides polonium (Po), thorium (Th), uranium (U), and radium (Ra) isotopes were measured in groundwater samples collected from different locations in the vicinity of the Waste Isolation Pilot Plant (WIPP) site in Carlsbad, New Mexico. The average values of gross activity concentrations of 210 Po, 228 Th, 238 U, 234 U, 226 Ra and 228 Ra isotopes were determined to be 1.62 Bq L -1 in shallow groundwater and 5.88 Bq L -1 in deep groundwater, respectively. The total radioactivity in deep groundwater was higher than that in shallow groundwater, and most of the radioactivity in the water is from 226 Ra. Furthermore, the effective doses for ingestion of natural radionuclides were about 0.333 mSv y–1 for shallow groundwater and about 1.338 mSv y –1 for deep groundwater samples, which are higher than the World Health Organization (WHO, 2017) guideline level (0.1 mSv y –1 ) for drinking water. Ra dominated the total ingestion dose, contributing 93.06 % and 75.40 % of the total effective doses to the deep and shallow groundwater, respectively. The ingrowth and decay of natural radionuclides suggested that 228 Ra/ 226 Ra ratio can be a useful indicator of the source of radioactive contamination. The radioactivity data obtained from the investigated groundwater samples can be used to establish a baseline for radioactivity levels in groundwater around the WIPP site.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Alpha Radiation Studies and Related Backgrounds in the DarkSide-50 Detector

DarkSide-50 is the current phase of the DarkSide direct dark matter search pro- gram, operating underground at the Laboratori Nazionali del Gran Sasso in Italy. The detector is a dual-phase argon Time Projection Chamber (TPC), designed for direct detection of Weakly Interacting Massive Particles (WIMPs), and housed within a veto system of liquid scintillator and water Cherenkov detectors. Since switching to a target of low radioactivity argon extracted from underground sources in April 2015, the background is no longer dominated by naturally occurring $^{39}$Ar. However, alpha backgrounds from radon and its daughters remain, both from the liquid argon bulk and internal detector surfaces. In some cases, the alpha events are a dangerous background in need of mitigation. In others, the alpha events can be used as a tool to deepen our understanding of our detector. We present here several analyses of alpha events in DarkSide-50. An analysis of radon-polonium coincidences is perfo rmed, yielding measurements of ion mobility and charged daughter fraction in liquid argon. These coincidences are also used to place upper limits on XY-resolution and liquid argon motion in the detector. A method for simulating the degraded energy spectra from $^{210}$Po events traveling through surface materials is presented and compared with data from DarkSide-50. Lastly, a pileup background created by the accidental coincidence of scintillation-only $^{210}$Po surface events with random ionization-like pulses is thoroughly discussed. The estimation of this background and its mitigation informed the recent WIMP search analysis performed with 532 live-days of DarkSide-50 data.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

210 Pb/ 210 Po isotope generator

As a continuation of previous work (Kmak et al. in J Radioanal Nucl Chem 314:985–989, 2017), an isotope generator column based on the 210 Pb decay chain has been made here to produce highly radiopure 210 Po. Two replicate studies were performed on AG 50Wx8 columns with an average yield of 90.4 ± 1.9%. 210 Pb breakthrough was seen at the 6 month elution for both generators.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

A Rapid Sequential Separation Method for Determination of Actinides and TENORM in Fracking Wastes - 20223

With recent advances in unconventional drilling technology in the US and around the world, the risks of environmental contamination and exposure due to technologically enhanced naturally occurring radioactive materials (TENORM) from fracking wastes have also surfaced. Although the Permian Basin (southeastern New Mexico, western Texas) has long been a modest producer of oil, the advent of fracking technology a decade ago turned it into hot property for producers. A 2018 assessment of undiscovered, technically recoverable continuous oil and gas resources by the U.S. Geological Survey estimates an average 46.3 billion barrels of oil and 281 trillion cubic feet of gas. This is likely to increase the use of unconventional drilling and TENORM generation. TENORM concentrations in oil and gas exploration and production waste can be several hundred to several thousand times higher than background TENORM concentrations. Both the thorium and uranium decay chains contribute to airborne radionuclides arising from the radon gas escaping the ground and subsequently decaying as airborne particulates. Additionally, radon decay products {sup 210}Pb and {sup 210}Po can build up in scale on the internal surfaces of oil and gas handling pipes and in sludge in refineries, becoming potential inhalation and ingestion hazards for workers. Furthermore, southeastern NM is also home to world's only licensed and operating transuranic nuclear waste repository, the DoE's Waste Isolation Pilot Plant (WIPP). Plutonium isotopes ({sup 239+240}Pu) and {sup 241}Am, are expected to account for more than 99% of the total radioactivity scheduled for disposal in the WIPP repository. Thus, an improved understanding of the environmental fate and transport of TENORM, liberated by unconventional drilling, is essential to assess how best to protect individuals and the environment. In this context, accurate measurement of TENORM and actinides in environmental and biological samples is essential. In this presentation, a new sequential method for the separation and pre-concentration of actinides (Pu, Am, Np) and TENORM (Po, U and Th) derived from oil and gas exploration is proposed. The TEVA method involves a rapid co-precipitation step to remove matrix interferences from the samples, followed by plutonium oxidation state adjustment to Pu (IV) and an incubation period of ∼ 1 hour at 50-60 deg. C to allow the resultant Po (II) to oxidize into Po(IV). The polonium, neptunium, thorium and plutonium are then separated on a TEVA column, while americium and uranium are separated on a TRU column. After separation, the alpha counting source was prepared by micro-precipitation with copper sulfide (CuS) for polonium and neodymium fluoride (NdF{sub 3}) for actinides. The efficiency and reliability of the procedures were tested by analyzing filter, drinking water and frack sand samples. The method is simple, robust and can be performed quickly with excellent removal of interferences, high chemical recovery and very good alpha peak resolution. (authors)

07 ISOTOPE AND RADIATION SOURCES↗