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DOE OSTI2025

Assessment of Hydroxyl Radical Reactivity in Sulfur-Containing Amino Acid Models Under Acidic pH

Methionine residues in proteins and peptides are frequently oxidized by losing one electron. The presence of nearby amide groups is crucial for this process, enabling methionine to participate in long-range electron transfer. Hydroxyl radical (HO•) plays an important role being generated in aerobic organisms by cellular metabolisms as well as by exogenous sources such as ionizing radiations. The reaction of HO• with methionine mainly affords the one-electron oxidation of the thioether moiety through two consecutive steps (HO• addition to the sulfur followed by HO− elimination). We recently investigated the reaction of HO• with model peptides mimicking methionine and its cysteine-methylated counterpart, i.e., CH3C(O)NHCHXC(O)NHCH3, where X = CH2CH2SCH3 or CH2SCH3 at pH 7. The reaction mechanism varied depending on the distance between the sulfur atom and the peptide backbone, but, for a better understanding of various suggested equilibria, the analysis of the flux of protons is required. We extended the previous study to the present work at pH 4 using pulse radiolysis techniques with conductivity and optical detection of transient species, as well as analysis of final products by LC-MS and high-resolution MS/MS following γ-radiolysis. Comparing all the data provided a better understanding of how the presence of nearby amide groups influences the one-electron oxidation mechanism.

Biochemistry & Molecular Biology↗

DOE OSTI2020

Shed Light in the DaRk LineagES of the Fungal Tree of Life—STRES

The polyphyletic group of black fungi within the Ascomycota (Arthoniomycetes, Dothideomycetes, and Eurotiomycetes) is ubiquitous in natural and anthropogenic habitats. Partly because of their dark, melanin-based pigmentation, black fungi are resistant to stresses including UV- and ionizing-radiation, heat and desiccation, toxic metals, and organic pollutants. Consequently, they are amongst the most stunning extremophiles and poly-extreme-tolerant organisms on Earth. Even though ca. 60 black fungal genomes have been sequenced to date, [mostly in the family Herpotrichiellaceae (Eurotiomycetes)], the class Dothideomycetes that hosts the largest majority of extremophiles has only been sparsely sampled. By sequencing up to 92 species that will become reference genomes, the “Shed light in The daRk lineagES of the fungal tree of life” (STRES) project will cover a broad collection of black fungal diversity spread throughout the Fungal Tree of Life. Interestingly, the STRES project will focus on mostly unsampled genera that display different ecologies and life-styles (e.g., ant- and lichen-associated fungi, rock-inhabiting fungi, etc.). With a resequencing strategy of 10- to 15-fold depth coverage of up to ~550 strains, numerous new reference genomes will be established. To identify metabolites and functional processes, these new genomic resources will be enriched with metabolomics analyses coupled with transcriptomics experiments on selected species under various stress conditions (salinity, dryness, UV radiation, oligotrophy). The data acquired will serve as a reference and foundation for establishing an encyclopedic database for fungal metagenomics as well as the biology, evolution, and ecology of the fungi in extreme environments.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Noninvasive Detection, Tracking, and Characterization of Aerogel Implants Using Diagnostic Ultrasound

Medical implants are routinely tracked and monitored using different techniques, such as MRI, X-ray, and ultrasound. Due to the need for ionizing radiation, the two former methods pose a significant risk to tissue. Ultrasound imaging, however, is non-invasive and presents no known risk to human tissue. Aerogels are an emerging material with great potential in biomedical implants. While qualitative observation of ultrasound images by experts can already provide a lot of information about the implants and the surrounding structures, this paper describes the development and study of two simple B-Mode image analysis techniques based on attenuation measurements and echogenicity comparisons, which can further enhance the study of the biological tissues and implants, especially of different types of biocompatible aerogels.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Remote Detection of Uranium Using Self-Focusing Intense Femtosecond Laser Pulses

Optical measurement techniques can address certain important challenges associated with nuclear safety and security. Detection of uranium over long distances presents one such challenge that is difficult to realize with traditional ionizing radiation detection, but may benefit from the use of techniques based on intense femtosecond laser pulses. When a high-power laser pulse propagates in air, it experiences collapse and confinement into filaments over an extended distance even without external focusing. In our experiments, we varied the initial pulse chirp to optimize the emission signal from the laser-produced uranium plasma at an extended distance. While the ablation efficiency of filaments formed by self-focusing is known to be significantly lower when compared to filaments produced by external focusing, we show that filaments formed by self-focusing can still generate luminous spectroscopic signatures of uranium detectable within seconds over a 10-m range. The intensity of uranium emission varies periodically with laser chirp, which is attributed to the interplay among self-focusing, defocusing, and multi-filament fragmentation along the beam propagation axis. Grouping of multi-filaments incident on target is found to be correlated with the uranium emission intensity. The results show promise towards long-range detection, advancing the diagnostics and analytical capabilities in ultrafast laser-based spectroscopy of high-Z elements.

42 ENGINEERING↗

DOE OSTI2021

Radiological Scouting, Monitoring and Inspection Using Drones

Human populations and natural ecosystems are bound to be exposed to ionizing radiation from the deposition of artificial radionuclides resulting from nuclear accidents, nuclear devices or radiological dispersive devices (“dirty bombs”). On the other hand, Naturally Occurring Radioactive Material industries such as phosphate production or uranium mining, contribute to the on site storage of residuals with enhanced concentrations of natural radionuclides. Therefore, in the context of the European agreements concerning nuclear energy, namely the European Atomic Energy Community Treaty, monitoring is an essential feature of the environmental radiological surveillance. In this work, we obtain 3D maps from outdoor scenarios, and complete such maps with measured radiation levels and with its radionuclide signature. In such scenarios, we face challenges such as unknown and rough terrain, limited number of sampled locations and the need for different sensors and therefore different tasks. We propose a radiological solution for scouting, monitoring and inspecting an area of interest, using a fleet of drones and a controlling ground station. First, we scout an area with a Light Detection and Ranging sensor onboard a drone to accurately 3D-map the area. Then, we monitor that area with a Geiger–Müller Counter at a low-vertical distance from the ground to produce a radiological (heat)map that is overlaid on the 3D map of the scenario. Next, we identify the hotspots of radiation, and inspect them in detail using a drone by landing on them, to reveal its radionuclide signature using a Cadmium–Zinc–Telluride detector. We present the algorithms used to implement such tasks both at the ground station and on the drones. The three mission phases were validated using actual experiments in three different outdoor scenarios. We conclude that drones can not only perform the mission efficiently, but in general they are faster and as reliable as personnel on the ground.

Pinto, Luís Ramos (ORCID:0000000319975484)↗

DOE OSTI2023

Impact of Glass Irradiation on Laser-Induced Breakdown Spectroscopy Data Analysis

Increased absorption of optical materials arising from exposure to ionizing radiation must be accounted for to accurately analyze laser-induced breakdown spectroscopy (LIBS) data retrieved from high-radiation environments. We evaluate this effect on two examples that mimic the diagnostics placed within novel nuclear reactor designs. The analysis is performed on LIBS data measured with 1% Xe gas in an ambient He environment and 1% Eu in a molten LiCl-KCl matrix, along with the measured optical absorption from the gamma- and neutron-irradiated low-OH fused silica and sapphire glasses. Significant changes in the number of laser shots required to reach a 3σ detection level are observed for the Eu data, increasing by two orders of magnitude after exposure to a 1.7 × 1017 n/cm2 neutron fluence. For all cases examined, the spectral dependence of absorption results in the introduction of systematic errors. Moreover, if lines from different spectral regions are used to create Boltzmann plots, this attenuation leads to statistically significant changes in the temperatures calculated from the Xe II lines and Eu II lines, lowering them from 8000 ± 610 K to 6900 ± 810 K and from 15,800 ± 400 K to 7200 ± 800 K, respectively, for exposure to the 1.7 × 1017 n/cm2 fluence. The temperature range required for a 95% confidence interval for the calculated temperature is also broadened. In the case of measuring the Xe spectrum, these effects may be mitigated using only the longer-wavelength spectral region, where radiation attenuation is relatively small, or through analysis using the iterative Saha–Boltzmann method.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

Recovering Density Fields inside Quasar Proximity Zones at z ~ 6

The matter density field at z ~ 6 is very challenging to probe. One of the traditional probes of the low density intergalactic medium that works successfully at lower redshifts is the Lyα forest in quasar spectra. However, at the end of reionization, the residual neutral hydrogen usually creates saturated absorption, thus much of the information about the gas density is lost. Luckily, in a quasar proximity zone, the ionizing radiation is exceptionally intense, thus creating a large region with nonzero transmitted flux. In this study we use the synthetic spectra from simulations to investigate how to recover the density fluctuations inside the quasar proximity zones. We show that, under ideal conditions, the density can be recovered accurately with a small scatter. We also discuss how systematics such as the quasar continuum fitting and reionization models affect the results. This study shows that by analyzing the absorption features inside quasar proximity zones we can potentially constrain quasar properties and the environments they reside in.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Could a Kilonova Kill: A Threat Assessment

Abstract Binary neutron star mergers produce high-energy emissions from several physically different sources, including a gamma-ray burst (GRB) and its afterglow, a kilonova (KN), and, at late times, a remnant many parsecs in size. Ionizing radiation from these sources can be dangerous for life on Earth-like planets when located too close. Work to date has explored the substantial danger posed by the GRB to on-axis observers; here we focus instead on the potential threats posed to nearby off-axis observers. Our analysis is based largely on observations of the GW170817/GRB 170817A multi-messenger event, as well as theoretical predictions. For baseline KN parameters, we find that the X-ray emission from the afterglow may be lethal out to ∼1 pc and the off-axis gamma-ray emission may threaten a range out to ∼4 pc, whereas the greatest threat comes years after the explosion, from the cosmic rays accelerated by the KN blast, which can be lethal out to distances up to ∼11 pc. The distances quoted here are typical, but the values have significant uncertainties and depend on the viewing angle, ejected mass, and explosion energy in ways we quantify. Assessing the overall threat to Earth-like planets, KNe have a similar kill distance to supernovae, but are far less common. However, our results rely on the scant available KN data, and multi-messenger observations will clarify the danger posed by such events.

Astronomy & Astrophysics↗

DOE OSTI2024

Charging, aggregation, and electrostatic dispersion of radioactive and nonradioactive particles in the atmosphere

Electrostatic dispersion can significantly impact the microphysical behavior of charged particles and ions until reaching zero space charge. However, although radioactive particles can be strongly charged in air, the influence of electrostatic dispersion has been neglected in understanding their behavior. This study is aimed at investigating the time evolution of the charge and size distributions of radioactive and nonradioactive particles in air and developing simple approaches for applications. With processes involving charging, aggregation, and electrostatic dispersion, a comprehensive population balance model (PBM) has been developed to examine particle charge/size distribution dynamics. It is shown that compared to nonradioactive particles, the charge and size distributions of radioactive particles may evolve differently with time because radioactivity and electrostatic dispersion can significantly affect the charging and aggregation kinetics of the particles. It is found that, after the Fukushima accident, background aerosols in the pathway of radioactive plumes might be highly charged due to ionizing radiation, suggesting that radiation fields may strongly influence in situ measurements of charged atmospheric particles. The comprehensive PBM is simplified, and then the verification and application of the simplified PBMs are discussed. This study provides useful insight into how radioactivity can affect the dynamic behavior of particles in atmospheric systems including radiation sources.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Regulatory Development Challenges and Opportunities for the Safe and Secure Transport of Radioactive Materials

Drafting regulations for transport safety and transport security achieve two separate objectives, which can lead to divergent outcomes. With transport safety, the principle goal is to protect the public and the environment from the effects of ionizing radiation, while in contrast, the principle goal of transport security is to protect the material from malicious actors. While many Member States may have transport safety regulations for radioactive materials, transport security regulatory development is still in its nascent stages globally. Trying to develop harmonized transport safety and transport security regulations could lead to challenges ranging from differences in terminology used in transport safety versus terminology uses in transport security, roles and responsibilities for the variety of stakeholders involved in transport, and finally, the possible role of multiple competent authorities in governing the transport of dangerous goods, which includes radioactive material. While the International Atomic Energy Agency (IAEA) is currently developing a process of a methodology for drafting transport security regulations, any process must address both safety considerations and security requirements. (As the most vulnerable part of the life cycle of radioactive materials, the need for harmonized transport safety/transport security regulations is essential.) This paper investigates the regulatory elements of the safety-security interface for nuclear and other radioactive material in transport. Examining challenges including use of terms, the role of multiple competent authorities, and practical challenges involved in the safe and secure transport of radioactive material, the paper analyzes the need for integrated regulatory development for the safe and secure transport of these materials.

Anderson, Kimberly↗

DOE OSTI2020

Analysis of RF high power sources for 1MW – range, 10 MeV CW industrial accelerator.

Cobalt-60 is the dominant source of ionizing radiation for sterilizing products in the $200B/year medical device industry. Security and accessibility concerns around this radioactive material - sourced from countries including Russia and China - present national security and economic risks. There is a continued national urgency to replace such high-risk sources with low-risk alternatives such as electron or x-ray beams driven by accelerators. While e-beam sources have been in use for many years, they still represent a small portion of the market. X-ray sources are becoming economical alternatives. Meeting the processing capacity required to replace Co-60 requires a step-change in the capability, efficiency, and overall operating cost of electron accelerators to make adoption feasible. The radiofrequency (RF) power that drives accelerating cavities represents significant capital and operating costs for these accelerators. For accelerator-based systems to be a viable alternative for these applications, RF systems must be economical to manufacture, deploy, and operate.

43 PARTICLE ACCELERATORS↗

DOE OSTI2021

Mastering Medaka Culture: Improved Techniques for Increasing Egg and Fry Production in Japanese Rice Fish ( Oryzias latipes )

Aquatic systems are integral to ecosystem function and human health. By trapping sediments and retaining nutrients, wetlands protect our water quality. However, a wetland’s capacity to trap sediments and nutrients also means they can capture many contaminants (e.g., heavy metals and radionuclides) released into the environment due to anthropogenic activities. Both heavy metals and radionuclides have detrimental effects on wildlife at acute dosages. However, little is known regarding underlying biological responses associated with chronic low dose exposure to both ionizing radiation and heavy metals. Our long-term research goal is to work to fill this knowledge gap using Medaka (Oryzias latipes), small fish amenable to experimental manipulation. However, the current study focused on altering the husbandry protocol of a laboratory colony of Medaka in a way that would increase colony size to at least 400 individual fish over a six-week period. At the beginning of our work, we followed a strict cleaning, feeding and egg harvesting protocol. Two weeks into our work, we suspected that food limitations may be negatively impacting egg production and noticed fungal growth on eggs. Thus, we altered the feeding regime and egg harvesting protocol. The altered protocol more than tripled egg production and almost doubled of fry production. By the end of our study the colony had 673 individuals: 191 adults and 482 fry. Furthermore, our protocol changes resulted in growth of the colony at sufficient numbers to begin experiments related to investigating sub-lethal impacts of heavy metals and radionuclides on Medaka.

Thompson, Melissa↗

DOE OSTI2021

Comparison of Attila Transport Code with MCNP in the Analysis of Small Modular Reactor Shielding

Of great importance in the design of a nuclear power plant is the evaluation of shielding from the ionizing radiation produced in the core of the nuclear reactor. This requires simulation software to predict the dose rates in the areas of interest. These problems are referred to as deep penetration problems, as they involve the reduction of a radiation field by two or three orders of magnitude or more. This makes accurate analyses difficult for Monte Carlo based solutions that rely on enough particles being sampled in an area of interest. Comparing the simulation of the same modeled system with more than one computer application, especially one that uses a different algorithmic approach, is a way to gain confidence in the results. In this research, two models were created, one in Monte Carlo N Particle (MCNP) which uses a stochastic algorithmic approach, and the other in Attila, which uses a deterministic algorithmic approach to test the validity of the model and to estimate the dose rates in the area of interest. Successful comparison of the two models is a way we can validate the model used for that estimation.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Superconducting Accelerators for High-Power X-ray production

To date, linear accelerators (linacs) as electron sources used to produce ionizing radiation for industrial purposes have been limited to less than 100 kW. When the electron beam is used directly, this is sufficient for most potential applications. However, when the electron beam is used for the production of photons (x-rays) which are then to be used in an application, this is not sufficient to compete with other sources of photons (gamma rays from cobalt-60). This paper will discuss acompact superconducting RF (CSRF) accelerator system that relies on emerging technologies that will be able to produce electron beam powers into the 100s of kW with efficiencies much better than present linacs. The focus is to produce x-ray beams for medical device sterilization to provide alternatives for the present use of cobalt-60 for this purpose.

43 PARTICLE ACCELERATORS↗

DOE OSTI2023

Impact of Actinide Complexation on Ligand Radiolysis

Although the actinides boast many unique physical and chemical properties, their inherent susceptibility to radioactive decay are what make them truly interesting elements to study. The absorption of ionizing radiation from actinide decay leads to the formation of a variety of transient and steady-state radicals, ions, and molecular radiolysis products that can lead to significant changes in the surrounding environment, and ultimately dictate steady-state actinide redox distributions and the longevity of molecules designed for actinide complexation. Radiolysis of the latter leads to complexant destruction and the concomitant formation of degradation products that can complicate actinide studies and processes. However, the radiation chemistry of most actinide complexants have been studied in the absence of the actinides they were designed to complex, which can lead to inaccurate conclusions on longevity and degradation product distributions, as metal ion complexation has been historically shown to influence a ligand’s radiolytic behavior. Consequently, bridging this knowledge gap is important for actinide science. Here, I will discuss the impact of actinide complexation on the steady-state and time-resolved radiation-induced reactivity of a variety of complexants, including, tributyl phosphate (TBP) and N,N,N',N'-tetraoctyl diglycolamide (TODGA) .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

The Role of Pulse Radiolysis in Advanced Nuclear Fuel Cycles

The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. The complexity and intensity of these effects are greatest during reactor operations and in the management of used nuclear fuel and waste. Radiation-induced processes typically promote the chemical transformation of molecules and materials with the formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of nuclear technologies. Consequently, a molecular-level understanding of radiation effects over multiple time, distance, and material domains is essential for the innovation and deployment of next generation nuclear technologies. Attaining this knowledge necessitates a firm grasp of radiation-induced reaction kinetics, for which pulsed electron radiolysis is the methodology of choice. Presented here are several recent studies from our group that demonstrate the critical role of pulsed electron radiolysis techniques in the advancement of our understanding of radiation-induced chemistry under advanced nuclear fuel cycle conditions. Research topics include late actinide redox chemistry, radiation robustness of used nuclear fuel reprocessing complexants, and the behavior of metal cations in high temperature molten salt media.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2022

High luminescence plastic scintillators

A plastic scintillator includes a polymeric matrix comprising a primary fluorophore capable of forming an amorphous glass in its pure form. The primary fluorophore is also capable of generating luminescence in the presence of ionizing radiation and includes: a central species including silicon; a luminescent organic group bonded to the central species or to an optional organic linker group, the luminescent organic group including fluorene or an analog thereof; and the optional organic linker group, if present, is bonded to the central species and the luminescent organic group.

Myllenbeck, Nicholas↗

DOE OSTI2023

High luminescence plastic scintillators

Myllenbeck, Nicholas↗