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At least 19 records

A Methodology for Determining the Concentration of Naturally Occurring Radioactive Materials in an Urban Environment

The detection of radioactive sources in an urban setting is greatly complicated by natural background radiation, which emanates from various materials including roadways, sidewalks, soil, and building exteriors. The method presented and demonstrated here represents an effort to characterize the concentration of naturally occurring radioactive material (NORM) in these types of materials. The location surveyed in this work was the Fort Indiantown Gap Combined Arms Collective Training Facility in Lebanon County, Pennsylvania. Over 70 measurements with a high-purity germanium detector were performed to ascertain the NORM concentrations present in the soil, asphalt, gravel, concrete, and walls found throughout the site. Monte Carlo radiation transport calculations were used to obtain detector responses for these various geometries and materials to convert these measurements into NORM concentration estimates. Lastly, synthetic spectra were simulated using the predicted source terms and compared to actual measurements, showing acceptable agreement.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Assessment of Naturally Occurring Radioactive Material (NORM) in Illicit Drugs Using High-Resolution Gamma Spectroscopy

This report documents results assessing the presence of Naturally Occurring Radioactive Material (NORM) in illicit drugs using high-resolution gamma spectroscopy. Specifically, high-purity germanium (HPGe) measurements were conducted at the Drug Enforcement Administration (DEA) South Central Laboratory on 11 samples (referred to as exhibits) including cocaine, fentanyl, heroin, ketamine, LSD, marijuana, methamphetamines, psilocybin mushrooms, and synthetic cannabinoids.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Precise Compositional Characterization of Plutonium Alloys by Electron Probe Microanalysis

Key Takeaway Points: • Unlike most other materials, the precise compositional analysis of plutonium, including compounds and alloys, is riddled by numerous difficulties that are unique to the element, including the high atomic number and radioactive nature. There’s work to be done! • Radioactive materials require special handling to ensure precise compositions can be measured by EPMA. • Mean Atomic Number background corrections are limited due to high average atomic number. • Mass Absorption Coefficients are unknown for most light elements. Quantification relies upon calibration curves. • Principal Component Analysis could be a useful tool to improve interpretation of complicated, multiple element X-ray maps.

Maner, IV, James L.↗

Measurement of the {sup 14}C Content in Liquid Scintillators by Means of a Small-Volume Detector in the Low-Background Chamber of the Baksan Neutrino Observatory

A setup for measuring natural-radioactivity backgrounds and ultralow concentrations of the isotope {sup 14}C in samples of a liquid organic scintillator was created at the low-background laboratory of the Baksan Neutrino Observatory (Institute for Nuclear Research, Russian Academy of Sciences) at a depth of 4900 mwe. The concentration of the radiocarbon {sup 14C} in a sample of a scintillator based on domestically produced linear alkylbenzene was measured, and it was found that {sup 14}C/{sup 12}C (3.3 ± 0.5) × 10{sup −17}.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radiation-chemical processes leading to origination and accumulation of oxygen in the Earth’s atmosphere

The role of natural radioactivity in the formation of the oxygen atmosphere of the Earth is discussed. The origination of oxygen in the free state in the hydrosphere and atmosphere is associated with the radiolysis of the water of the World ocean under the irradiation of radio active isotopes {sup 40}K, {sup 235}U, {sup 238}U, and {sup 232}Th. The calculations showed that within the last 3.8 billion years the total weight of oxygen, which could be formed due to this process, is about 7.4•10{sup 17} kg, i.е., the value of the same order as the oxygen content in the modern atmosphere of the Earth. The Ocean was an intermediate collector and provided the nucleation of new forms of biological life with oxygen respiration. The consecutive transformation of the Earth’s atmosphere with a gradual increase in the oxygen content became the result of photosynthesis in algae and green plants and thus opened a way to the origination of complicated forms of the life.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Approaches for Communicating Technical Information - 16012

Projects within the nuclear industry are generally complex and associated with high hazards. To achieve success there is often a necessity to apply innovation or adopt longer term strategies and solutions. Because of these long timescales and the fact that some approaches revolve around allowing natural radioactive decay to take place prior to visible action, the industry is sometimes perceived to be technically unable to make progress with its environmental and waste management obligations. Work within the industry additionally takes on a high profile and invariably creates greater levels of anxiety and mistrust in the eyes of stakeholders than comparable projects from non-nuclear related industries. Many aspects of the industry are still seen as secretive, environmentally detrimental and 'risky' and all components of the nuclear life-cycle are therefore open to external scrutiny. Although communication and engagement has increased greatly over the years, especially in developed countries, there is still room for improvement in this field. Such improvement might relate to the frequency and level of engagement, the subject matter or the actual process itself. Communication with stakeholders is required throughout the various phases of the nuclear lifecycle whether the activity relates to mining/milling of uranium, fuel production, operational plant activities, decommissioning, remediation or waste management. The concerns and aspirations of stakeholders during these different activities will vary but need to be adequately addressed. Some organisations now have a basic engagement program and convince themselves that they are carrying out true engagement. But just ticking a box to say that an engagement program is in place does not provide evidence of its appropriateness or success as on many occasions' organisations might still not understand how to adequately engage and communicate technical information. It is not always the information we choose to communicate but that which might be withheld that is often perceived to be most relevant to the stakeholder community. Communicating technical information isn't as straightforward as it sounds, but still has to be undertaken, otherwise trust, understanding and acceptance of chosen options will not be achieved. I utilise what I call the 'ten principles of engagement' which I believe can help when communicating technical Information in relation to nuclear and radiological matters. These are; 1. Develop Trust. 2. Educating people and providing information in a transparent manner. 3. Develop an engagement process that is truly a two way process. 4. Openly discuss risk perception and risk communication. 5. Never try to trivialise risk. 6. Where possible, simplify the language you use. 7. Put background and naturally occurring radioactivity into context. 8. Explain how radioactive materials are often used in everyday life. 9. Try to demonstrate that you too are a member of the public. 10.Walk the talk - Try to undertake what you wish others to undertake. Further research is being undertaken to determine if Mental Models might assist with the communication of nuclear and radiological information. A mental model is an explanation of someone's thought process about how something works in the real world. The mental model approach aims to investigate the judgment and decision-making processes of both expert and lay groups, thus allowing a comparison and visualisation of the different views to be made. It is undoubtedly worthwhile keeping a watching brief on the outcome of such research as we strive to improve our communication with the general public. The aim of this paper is to highlight some simple principles and approaches that can assist with the communication of technical information. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Measurements of Argon-39 from locations near historic underground nuclear explosions

Measurement of radioactive gas seepage from an underground nuclear explosion is one of the primary methods to confirm whether an event was nuclear in nature. Radioactive noble gas indicators that are commonly targeted by such measurements (e.g. 133Xe, 37Ar) have half-lives of 35 days or less. Argon-39, an activation product similar to 37Ar, is produced by the interaction between neutrons and potassium in the surrounding geology and has a half-life of 269 years. Measurements taken at three sites near three historic underground nuclear test locations at the Nevada National Security Site have all shown highly elevated levels of 39Ar in subsurface air decades after the test events. Elevated levels of 39Ar (30-50 times background) were also detected in atmospheric air collected roughly 30 cm above ground level near two of these sites, and outside the entrance of the one tunnel site. These measurements demonstrate that 39Ar has the potential to be a long-term signature of an underground nuclear event which can be reliably detected at the surface or in the shallow subsurface. This radionuclide detection of an underground nuclear event decades after the event takes place is in contrast to the commonly held assumption that detecting underground nuclear events via radionuclides at the surface needs to be done in a matter of months. Depending upon what further studies show about the robustness of this signature in a variety of geological settings, it may in fact be easy to detect underground nuclear events at the surface for a very long time post-detonation.

Johnson, Christine M.↗

Health effects of Radiation and Radioactivity + Historic Nuclear Accidents

The safety of nuclear energy technology goes hand in hand with a modern understanding of the health impacts and required precautions associated with radiation. This is because nuclear power plants require fuel sources like uranium, which is an element that is naturally radioactive.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Subsurface cosmogenic and radiogenic production of 42 Ar

Radioactive decays from 42 Ar and its progeny 42 K are potential background sources in large-scale liquid-argon-based neutrino and dark matter experiments. In the atmosphere, 42 Ar is produced primarily by cosmogenic activation on 40 Ar. The use of low radioactivity argon from cosmogenically shielded underground sources can expand the reach and sensitivity of liquid-argon-based rare event searches. We estimate 42 Ar production underground by nuclear reactions induced by natural radioactivity and cosmic-ray muon-induced interactions. At 3,000 mwe, 42 Ar production rate is 1.8×10 -3 atoms per ton of crust per year, 7 orders of magnitude smaller than the 39 Ar production rate at a similar depth in the crust. In conclusion, by comparing the calculated production rate of 42 Ar to that of 39 Ar for which the concentration has been measured in an underground gas sample, we estimate the activity of 42 Ar in gas extracted from 3,000 mwe depth to be less than two decays per ton of argon per year.

07 ISOTOPE AND RADIATION SOURCES↗

Tank Waste Characterization: History, Challenges, and Success Stories

The preparation and chemical and radiochemical analysis of Hanford tank waste samples can be performed with standard laboratory equipment and instruments as relatively routine processes that are not particularly challenging. Rather, the main challenges of tank waste characterization are associated with radiological dose and sampling limitations. Accurate, representative and effective sampling techniques are difficult with the waste tanks because they were not designed for routine sampling. There are a finite number of sampling locations for each tank based on riser positioning, depth and the operational functionality of the sampling riser. For example, in one recently emptied SST, there was one riser that was found to have had concrete dumped down it, thereby eliminating that sampling port. Additionally, the waste within the tank; especially true for the saltcake and sludge, is not homogenous. The ability to adequately mix a million-gallon double shell tank (DST) is a concern for data reproducibility. Another real challenge that must be addressed for sampling single shell tanks, is how to dissolve the salt cake waste in a compromised (leaking) SST. These physical constraints mean that uncertainty in the representativeness of samples must be considered when applying analytical results to the bulk contents of the tank. The tank waste is highly radioactive and thus can only be handled initially by facilities that can receive samples into concrete-shielded hot cells with remote operation with an example provided in Figure 1. The shielding protects the worker from the radiological dose while mineral oil windows and remotely operated manipulators enables the samples to be handled. At Hanford, analytical laboratories with these hot cell capabilities are limited to the Pacific Northwest National Laboratory and the main Hanford operations support laboratory, 222-S Laboratory. Because of their highly radioactive nature, samples must be sufficiently diluted to facilitate their analysis outside of a shielded cell. In some cases, this means some accuracy must be compromised to complete the analysis beyond that normally encountered for non-radioactive material.

Waste Characterization, BBI, PHOENIX: Tank Farms: ↗

Probing electronic structure in berkelium and californium via an electron microscopy nanosampling approach

Due to their rarity and radioactive nature, comparatively little is known about the actinides, particularly those with atomic numbers higher than that of plutonium, and their compounds. In this work, we describe how transmission electron microscopy can provide comprehensive, safe, and cost-effective characterization using only single nanogram amounts of highly-radioactive, solid compounds. Chlorides of the rare elements berkelium and californium are dropcast and then converted in situ to oxides using the electron beam. The f-band occupancies are probed using electron energy loss spectroscopy and an unexpectedly weak spin-orbit-coupling is identified for berkelium. In contrast, californium follows a jj coupling scheme. These results have important implications for the chemistries of these elements and solidify the status of californium as a transitional element in the actinide series.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Identification of Distorted Gamma-Ray Signature Patterns Using Digital Filtering and Auto-Associative Memory Implemented with a Hopfield Neural Network

The detection and identification of radioactive sources in search applications involve analyzing passive gamma-ray emissions from high-level radioactive materials. This process uses a mobile detector-spectrometer in a complex field test environment. Recently, the use of artificial intelligence for gamma-ray spectrum analysis has shown promising results. However, challenges persist in identifying isotopic signatures from spectral measurements that may be distorted due to source shielding, random variations in natural radioactive background, or insufficient measurement time to obtain clear spectral lines. Here, this paper presents a novel intelligent signature recognition method that combines digital filtering techniques with an artificial Hopfield Neural Network (HNN). The HNN leverages auto-associative memory to store training sample patterns and match them with incoming gamma spectra from distorted sources. It restores the testing sources’ measurements by finding the closest matching signature patterns in the spectral library. Before HNN recognition, the measured spectrum undergoes preprocessing with a digital image filter to reduce fluctuations. Performance of the proposed method is evaluated using a set of gamma-ray spectra measured with a sodium iodide detector. The data collected include measurements from six pure samples: 241 Am, 60 Co, 137 Cs, 192 Ir, 239 Pu, and 235 U, which are used for training and validation (i.e. six cases). Additionally, the data set contains 24 distorted synthesized sources with various fluctuating backgrounds. Test results demonstrate the potential of the proposed method to accurately recognize the correct isotope with high precision, achieving an accuracy rate exceeding 85%. Furthermore, the proposed method exhibits superior performance compared to the conventional multiple regression fitting and simple feedforward neural network methods.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Structural Properties of Ditechnetium Heptoxide, Tc{sub 2}O{sub 7}

Group 7 elements form unique binary oxides with the stoichiometry M{sub 2}O{sub 7}. The heptoxides of manganese and technetium crystallize as molecular solids while rhenium forms an extended solid with mixed valances, 4 and 6. Unlike manganese and rhenium heptoxides which are used in the chemical industry technetium heptoxide has found very few applications due to its radioactive nature; it has been primarily use as a chemical precursor. While both of the molecular solids, Mn{sub 2}O{sub 7}{sup 3} and Tc{sub 2}O{sub 7}{sup 4} can be described by two corner-sharing MO{sub 4} tetrahedron. The most distinctive difference is that the manganese's compound has a metal-oxygen-metal bond angle of 120.7 deg. while the technetium species is 180 deg.. Additionally, Tc{sub 2}O{sub 7} has the largest molar volume of the heptoxides which suggest that it will be more susceptible to external stimuli of pressure and temperature than the others heptoxides. A pressure induced twisting has been predicted by Fang et al. Anomalous behavior is seen in the c-axis where below 2 GPa the Van der Waals interactions between the Tc{sub 2}O{sub 7} molecules is over come and compression is observed but at higher pressures the twisted distortion forces the lattice to expand. The terminology diagonal-double tetrahedrons (DDTs) is introduced to discuss the molecules of Tc{sub 2}O{sub 7}. The rigid nature of the DDTs has been attributed to the cause of this twisted distortion mechanism. Recently, the solid state and gas phase behavior of technetium heptoxide was revisited by Childs et al. in light of {sup 99}Tc being an important dose contributor in the Hanford waste and vitrification being proposed for immobilization of nuclear waste. Technetium heptoxide is one of the proposed volatilized species of technetium found in the vitrification process. In this study the crystal structure of Tc{sub 2}O{sub 7} was reported at 100 K and compared to the structure first determined by Krebs at room temperature. Inspection of the metal-oxygen distances revealed the 100 K structure had longer bond lengths for the bridging oxygen than at high temperature. It is suggested that transverse thermal vibrational modes can be used to explain this negative thermal expansion behavior. This describes the average bond length of a central atom (i.e. the bridging oxygen atom) being measured as shorter at higher temperatures due to the larger thermal motion. Diffraction methods that measure the long range average structure are susceptible to observing this shorter average length as opposed to the true bond length, atom position at oscillation node that a method like Pair-Distribution Functional PDF Analysis would yield. In the case of Tc{sub 2}O{sub 7}, the magnitude of the transverse thermal vibrational mode is at the limit of being detectable by SCXRD and likely not observable by PDF analysis. Here we report the preliminary results of our study on the nature of the thermal expansion behavior of Tc{sub 2}O{sub 7}. The transverse thermal vibration mode compression mechanism is considered and compared to the pressure induced twisted distortion mechanism predicted at high pressure. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Investigating radioactive negative ion production via double electron capture

The relative cross sections for radioactive negative ion production via double electron capture have been measured for collisions between a 40 keV projectile beam of uranium-238 and potassium vapor. This was performed at the collinear resonance ionization spectroscopy (CRIS) experiment at CERN-ISOLDE and is a step towards measuring the electron affinities (EAs) of elements that cannot be efficiently produced in negative ion sources at radioactive ion beam (RIB) facilities. This includes short-lived radioactive isotopes that have low production quantities and heavy and superheavy elements that systematically have smaller EAs than work functions of available ion source materials. Negative ions are particularly sensitive to electron–electron correlation effects, which make such studies ideal for benchmarking atomic structure models that go beyond the independent particle model. While the EAs of most light elements have been measured, experimental investigations on heavier elements, namely the actinides, remain scarce due to their radioactive nature and production difficulty. By developing negative ion production by charge exchange, we aim to make these studies feasible at RIB facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Understanding Materials Characteristics of Palladium Lanthanide Cermet Wires as a Mimic of Californium Wire Production

Californium-252 (Cf-252) has been synthesized on a large scale (mg) since the 1970s for use as a portable neutron source. With a half-life of 2.645 years and a spontaneous fission fraction of 3.09%, Cf-252 emits 2.31 × 10 12 neutrons/gram second. Today most of the Cf-252 produced in the world is made at Oak Ridge National Laboratory (ORNL) using the High Flux Isotope Reactor (HFIR) and the Radiochemical Engineering Development Center (REDC). Because of its highly radioactive nature, all manipulations of Cf-252 need to be performed in hot cell facilities by highly trained personnel. The Cf-252 produced at ORNL is done at the REDC, which is conveniently located next to the HFIR. Cf-252 is sold as bulk wire, which has been described as palladium (Pd) metal incasing californium oxide (Cf 2 O 3 ). The process was developed by Mosley et al. at Savannah River Laboratory (SRL) where it was modeled after the thorium work done by Fuschillo et al. This process has been used since the 1970s to synthesize this unique wire, but its fundamental chemistry and materials characteristics were never openly reported. Here we aim to better understand the chemistry and the materials characteristics of Cf-252 wire production for process improvements and to better our fundamental understanding of the mid-late actinides. Though there are many challenges in working with radioactive elements such as Cf, the isotope Cf-252 is even more complicated due to its neutron emission. One challenge with neutron emission is the ability of neutrons to penetrate much deeper through materials, causing radiation damage. This makes using instrumentation to characterize the chemistry and materials properties of this process difficult. For this reason, this study will first focus on terbium (Tb) as a surrogate for Cf. Currently Tb is used as a carrier or filler in Cf production when small amounts of Cf are being processed. This, along with their similar size and charge, makes Tb a reasonable surrogate for this study.

36 MATERIALS SCIENCE↗

Concept of an upright wearable positron emission tomography imager in humans

Abstract Background Positron Emission Tomography ( PET ) is traditionally used to image patients in restrictive positions, with few devices allowing for upright, brain‐dedicated imaging. Our team has explored the concept of wearable PET imagers which could provide functional brain imaging of freely moving subjects. To test feasibility and determine future considerations for development, we built a rudimentary proof‐of‐concept prototype (Helmet_ PET ) and conducted tests in phantoms and four human volunteers. Methods Twelve Silicon Photomultiplier‐based detectors were assembled in a ring with exterior weight support and an interior mechanism that could be adjustably fitted to the head. We conducted brain phantom tests as well as scanned four patients scheduled for diagnostic F 18‐ FDG PET / CT imaging. For human subjects the imager was angled such that field of view included basal ganglia and visual cortex to test for typical resting‐state pattern. Imaging in two subjects was performed ~4 hr after PET / CT imaging to simulate lower injected F 18‐ FDG dose by taking advantage of the natural radioactive decay of the tracer (F 18 half‐life of 110 min), with an estimated imaging dosage of 25% of the standard. Results We found that imaging with a simple lightweight ring of detectors was feasible using a fraction of the standard radioligand dose. Activity levels in the human participants were quantitatively similar to standard PET in a set of anatomical ROI s. Typical resting‐state brain pattern activation was demonstrated even in a 1 min scan of active head rotation. Conclusion To our knowledge, this is the first demonstration of imaging a human subject with a novel wearable PET imager that moves with robust head movements. We discuss potential research and clinical applications that will drive the design of a fully functional device. Designs will need to consider trade‐offs between a low weight device with high mobility and a heavier device with greater sensitivity and larger field of view.

60 APPLIED LIFE SCIENCES↗

Radiogenic backgrounds in the NEXT double beta decay experiment

Natural radioactivity represents one of the main backgrounds in the search for neutrinoless double beta decay. Within the NEXT physics program, the radioactivity-induced backgrounds are measured with the NEXT-White detector. Data from 37.9 days of low-background operations at the Laboratorio Subterr\'aneo de Canfranc with xenon depleted in $^{136}$Xe are analyzed to derive a total background rate of (0.84$\pm$0.02) mHz above 1000 keV. The comparison of data samples with and without the use of the radon abatement system demonstrates that the contribution of airborne-Rn is negligible. A radiogenic background model is built upon the extensive radiopurity screening campaign conducted by the NEXT Collaboration. A spectral fit to this model yields the specific contributions of $^{60}$Co, $^{40}$K, $^{214}$Bi and $^{208}$Tl to the total background rate, as well as their location in the detector volumes. The results are used to evaluate the impact of the radiogenic backgrounds in the double beta decay analyses, after the application of topological cuts that reduce the total rate to (0.25$\pm$0.01) mHz. Based on the best-fit background model, the NEXT-White median sensitivity to the two-neutrino double beta decay is found to be 3.5$\sigma$ after 1 year of data taking. The background measurement in a Q$_{\beta\beta}\pm$100 keV energy window validates the best-fit background model also for the neutrinoless double beta decay search with NEXT-100. Only one event is found, while the model expectation is (0.75$\pm$0.12) events.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Selenium interaction with iron minerals: Quantitative comparison of sorption and coprecipitation impacts on mobility

Given the significance of selenium (Se) as a micronutrient, the radioactive nature of some of its isotopes, and its affinity to iron (Fe) minerals, extensive research has been conducted on the sorption mechanisms between Se and these minerals. Here, in this study, we employ sorption data sourced from the L-SCIE database and coprecipitation data from available literature to achieve the following objectives: i) establish coherence between adsorption and coprecipitation processes, ii) quantitatively evaluate the importance of these processes in nuclear waste repository science, and iii) propose a forward-looking approach for integrating coprecipitation into reactive transport models. Our findings indicate that a correlation between Se adsorption and coprecipitation can be established using the λ formalism. The comparable log(λ Se(IV) /λ Se(VI) ) ratios derived from adsorption and coprecipitation experiments suggest that these processes can be quantitatively compared and evaluated using our numerical approach. Across all iron oxide phases examined, coprecipitation leads to significantly greater immobilization of Se compared to adsorption. Specifically, for hydrous ferric oxide, hematite, and goethite, coprecipitation is predicted to result in 100–1000 times more Se immobilization compared to adsorption, irrespective of the Se oxidation state (Se(IV) or Se(VI)); notably stronger immobilization potential via coprecipitation was observed for magnetite. The modeling approach and quantitative analysis presented herein clearly highlight the importance of including coprecipitation processes when simulating Se (and other elements) transport, particularly under conditions where mineral compositions are transient or evolving with time. Neglecting coprecipitation in models is likely to lead to significant overestimates of migration.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗