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At least 109 records · Page 6

Testing the Jump Finding Code for NEXUS Qubit Analysis

At Fermilab, the NEXUS dilution refrigerator is repeating the same experiment from Wilen et al. 1 underground to further investigate the effect of ionizing radiation and cosmic ray muons on qubit decoherence. This refrigerator is 100m underground in the MINOS cavern to significantly lower the incident rate of cosmic ray muons, meaning the majority of incidents is due to ionizing radiation. To gain a better understanding of how the rate of ionizing radiation affects the qubits, we use 4 radiation configurations to collect data from the chip. In this work, we examine the efficiency of our jump detection code to find jumps of various sizes. We do so using simulated data with a known number of injected jumps of known sizes. These jumps are charge offsets of the qubit, thought to be due to quasiparticle poisoning. To test this, we run the jump finding code on an array of simulated data in which two main parameters, the smoothing factor and the threshold at which a charge offset is considered a jump, are changed to test an array of these parameters. We then perform a χ2 analysis to find the best combination of these two parameters.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Unravelling the radiation-induced redox chemistry of plutonium ions in aqueous solution

Plutonium plays a critical role in nuclear fuel cycle technologies, but our understanding of its fundamental radiation-induced redox chemistry is limited. Changes in oxidation states affect the speciation and transport of plutonium ions in solution. For example, solvent extraction techniques used to separate and recover plutonium from used nuclear fuel rely on the selective formation, maintenance, and complexation of specific plutonium oxidation states. However, radiolytically generated radicals, ions, and molecules can drive the oxidation state distribution of plutonium ions far from equilibrium, ultimately changing the physical and chemical properties of the bulk system. These radiation-induced processes are inevitable due to the ionizing radiation fields generated by the radioactive decay of plutonium and its daughter nuclides. Therefore, mechanistically understanding how plutonium's various oxidation states respond to ionizing radiation is essential for predicting its behavior in solution. Here, we present significant advances in our understanding of radiation-induced plutonium redox chemistry by using time-resolved (electron pulse) and dose accumulation (alpha and gamma) irradiation techniques, along with quantitative multiscale modeling methods.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

A Radiation-Shielded, Shallow Underground, Long-Coherence Time Quantum Qubit Concept

Ionizing radiation from ambient radioactivity has been shown to reduce the coherence time of superconducting qubits. Qubit performance can be improved by shielding the system from external radiation: operating the system underground to reduce cosmic rays, and use of lead shielding to reduce ambient gammas. Here we present a design for a lead shield optimized for a dilution refrigerator operating in PNNL's Shallow Underground Laboratory. The shield reduces the ambient gamma flux by approximately 99.8%, so that cosmic ray muons dominate the ionizing radiation input to the qubits.

42 ENGINEERING↗

Impact of trivalent f-element complexation and chemical environment on the radiation-induced chemical reactivity of TODGA and HOPO ligands

Understanding the impact of ionizing radiation on ligands employed and proposed for the separation, recovery, and transport of actinide ions is of vital importance for the innovation of nuclear fuel cycle technologies. In the presence of ionizing radiation fields, complexing ligands are subject to radiolytic processes, that lead to their destruction and the formation of potentially detrimental degradation products. Consequently, mastery of the radiation-induced behavior of these ligands is essential for predicting and optimizing their effectiveness, longevity, and minimizing the negative impacts of radiolysis. Furthermore, this knowledge is critical for the design of more radiation resistant molecules to be incorporated into advanced separation technologies. That said, the radiation chemistry of most actinide complexants have only been studied in the absence of their targeted metal ion complexes, which can lead to inaccurate conclusions on their radiolytic robustness and impacts on performance. With this in mind, we present our findings on the impact of f-element complexation and chemical environment on the radiation-induced chemical reactivity of N,N,N',N'-tetraoctyl diglycolamide (TODGA) and the model octadentate hydroxypyridinone ligand 3,4,3-LI(1,2-HOPO) (abbreviated as HOPO), both promising candidates for actinide separations

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Elucidating the Radiation-Induced Redox Chemistry of Plutonium Under Used Nuclear Fuel Reprocessing Conditions

Plutonium plays a critical role in the development of sustainable nuclear fuel cycles, and yet, our fundamental understanding of this element’s inherent radiation-induced redox chemistry and associated impacts on nuclear fuel cycle technologies is limited. Unanticipated changes in oxidation state distribution can influence the speciation and transport of plutonium in a given process. Control of these parameters is especially important for used nuclear fuel reprocessing technologies, wherein the separation and recovery of plutonium is typically achieved by the selective formation, maintenance, and complexation of specific oxidation states. Furthermore, plutonium’s inherent radiation-induced redox chemistry has the capacity to influence the radiolytic behavior of its complexes, the longevity of which are critical in the design of efficient and cost-effective advanced reprocessing technologies. These radiation-induced processes are unavoidable under fuel cycle conditions owing to the inherency of ionizing radiation fields to the decay of plutonium’s isotopes and to the various other radioisotopes generated by nuclear fission and neutron-capture process and the subsequent radioactive decay of their products. As such, mechanistically understanding the response of plutonium’s multiple oxidation states to multi-component ionizing radiation fields is essential for predicting the behavior of this critical element under used nuclear fuel reprocessing conditions. Here, through a combination of time-resolved (electron pulse) and steady-state (alpha and gamma) irradiation experiments complemented by quantitative, multiscale modeling calculations, we present advances in our understanding of radiation-induced plutonium redox chemistry!

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Understanding Radiotropism in Filamentous Fungi

Melanized species of filamentous fungi isolated from high radiation environments have been reported to exhibit radiotropism, defined as the directed growth toward a source of ionizing radiation. Inconsistencies in the experimental approaches and results have impeded our understanding of the key factors involved in radiotropism. In the present study, we assessed radiotropism in four isolates of fungi: Aspergillus niger, A. calidoustus JC-1043, Paecilomyces variotii SNL-1, and P. variotii IMV-00236. Of these fungi, only P. variotii IMV-00236 had been previously reported to exhibit radiotropic behavior. Plates of each fungus were placed in equivalent proximity to a 137 Cs source, with a primary gamma emission of 662 keV, and differences in the rate and direction of mycelia growth were measured over a seven-day period. Significant differences were not observed in the rate or direction of growth of the different fungi based on exposure to gamma radiation, which suggested a lack of measurable radiotropism in these experiments. Additional studies varying parameters such gamma emission rates and energies, as well as other types of ionizing radiation (e.g., alpha and beta particles, neutrons) are necessary to gain further insights to the factors critical to the expression of radiotropic behavior in filamentous fungi.

59 BASIC BIOLOGICAL SCIENCES↗

Radiation-induced transients on solid and molten Li and K iodides

The study, quantification, and monitoring of iodine in nuclear power generation systems have been paramount due to its environmental and health implications. Thorough speciation and transport studies strengthened the development and deployment of water reactors, which are now required for the new generation of Molten Salt Reactors (MSR), where the fuel and coolant are a complex liquid system of suitable halides. The speciation, radiation-induced chemistry, and transport of iodine (I-127, I-129 and I-131) under extreme conditions of temperature and ionizing radiation are among the challenges for the future implementation of MSR’s. In aqueous systems, the triiodide-iodine-iodide (I3--I2-I-) equilibrium is strongly dependent on the conditions of the medium. In molten iodides and chlorides, the triiodide detection (and its disproportionation) poses challenges due to the extreme conditions of temperature and radiation, but studies have shown a dependence on temperature, absorbed dose and salt composition. Through absorption spectroscopy techniques (diffuse reflectance and high-temperature UV-Vis), as well as resonance (Electron Paramagnetic Resonance) it is possible to identify primary transients induced by ionizing radiation trapped in the solid phase (Solid-state radiolysis), and steady-state main absorption components with a fast-acquisition real-time spectroscopy. The presence of heterogeneous phase (colloids), viscosity changes, and gas evolution are among the observed processes. A specific case of study is speciation in the presence of Ni. A corrosion product with magnetic properties due to unpaired electrons in its electronic structure. Ferromagnetic materials are monitored in solidified salts to identify aggregation and phase separation. Comparative studies of eutectic mixtures of LiI-KI and LiCl-KCl with known addition of dopants will be presented, with a perspective of radiation chemistry and its possible implications in complex systems.

36 - MATERIALS SCIENCE↗

Strong ultrafast nonlinear optical response from megaelectronvolt electrons in semiconductors

Understanding radiation–matter interactions on ultrafast timescales is essential for radiation detection technologies, particularly those requiring precise timing, such as plasma monitoring, synchrotron diagnostics and medical imaging. However, the detection of highly ionizing radiation is challenging due to the stochastic nature of the interactions, resulting in dispersed energy deposition. Here we show a nonlinear optical response in semiconductors induced by 150-fs, 4.2-MeV electrons that generate highly localized charge carriers. The induced sub-10-ps optical modulation reached up to 24.5%, accompanied by a blueshift in the absorption edge consistent with band filling and carrier densities of 10 18 cm −3 . These carrier densities are 100-fold higher than expected from the deposited energy, indicating the extreme spatial localization of carriers at inelastic collisions along the ionization trajectories, thereby leading to the observed modulation. The strong nonlinearity of the MeV-electron-induced optical response enables the precise spatiotemporal detection of ionizing radiation at room temperature using common semiconductors and laser systems.

Jeong, D. [Stanford Univ., CA (United States)] (OR↗

Updates to Composite Analysis Base Case and Null Space Monte Carlo Sensitivity Based on New Unit Dose Factors

This environmental calculation file (ECF) presents the results of the exposure route-specific and total radiological dose assessments for the groundwater exposure pathway as a part of the updated Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2022), based on revised unit dose factors (UDFs) published in CA Special Studies: Updates to the Groundwater Pathway Radiological Dose. The reason for these radiological dose assessments is to estimate the cumulative radiological impacts from all screened sources of ionizing radiation and exposure routes that could potentially contribute to the projected dose to a hypothetical member of the public. Sources of ionizing radiation can include existing or future disposal facilities and other sources including past-practice discharge sites. Additionally, the results of the exposure route-specific and total radiological dose assessments have been revised for the groundwater pathway based on the null space Monte Carlo (NSMC) groundwater concentrations and the most recent updates to the UDFs as a part an uncertainty analysis for the updated Hanford Site CA.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Dodecane Radiolysis Yields by Time-Resolved and Steady-State Methods

Liquid organic molecules are present as solvents, complexing ligands, and additives in both used nuclear fuel reprocessing solvent systems and in their subsequent nuclear waste streams. Under these extreme environments, these organic molecules are constantly exposed to ionizing radiation which promotes their radiolysis, forming a variety of short-lived, highly energetic, excited state and radical species.1-4 Here, we demonstrate new experimental results for the steady-state and time-resolved irradiations of dodecane (C12H26), a long chain, liquid, aliphatic hydrocarbon that is the prototypical solvent used for benchtop studies of aqueous-organic solvent extraction systems. When ionizing radiation interacts with neat dodecane, the energy transfer can result in molecular ionization, to give the dodecane radical cation (C12H26+•) and the solvated electron (eS–), and molecular electronic excitation (C12H26*), which rapidly produces transient carbon-centered radical fragments (CxHy•) and hydrogen atoms (H•).1-4 Studies on the initial yields of the ionization and excitation products were performed using time-resolved picosecond electron pulse radiolysis with the use of molecular probes. Using steady-state cobalt-60 gamma irradiations, the suite of products formed by dodecane radiolysis in aerated and deaerated solutions was determined. Then, using iodine as an alkyl radical scavenger, the loss of molecular iodine with dose was quantified, and by correlating with the molecular hydrogen yields of the system, the initial yields of the various carbon-centered radicals were also determined. Finally, the rates of reactions of the C12H26+• and eS– with ligands proposed for use in spent nuclear fuel reprocessing were studied as a function of temperature from 10 – 40 °C.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗

Radiation-induced dry reforming: A negative emission process

The reaction between the most abundant greenhouse gases (GHG) to produce hydrogen might represent the most powerful and effective decarbonizing opportunity, if a low-carbon energy source is used to drive it. This is the case of methane (CH 4 ) dry reforming (MDR) where its reaction with carbon dioxide (CO 2 ) produces synthesis gas (syngas, a mixture of carbon monoxide and hydrogen). Here this study explores the feasibility of using ionizing radiation to induce the MDR reaction, at low temperatures and/or less energy demanding conditions. Additionally, the ionizing radiation is proposed to be supplied by nuclear power plants (NPPs), which are low-carbon reliable energy generation sources. Thus, the radiolysis of CO 2 , CH 4 and their mixtures, under ?-irradiation was evaluated in the absence and presence of nickel catalysts. The radiation-induced MDR reaction and radiation-induced catalytic promotion were proven to take place at temperatures close to ambient though at low conversion, with yields below 1%. Since irradiation and heat can be provided by a nuclear power plant, this radiation-induced reaction establishes a connection between nuclear energy to renewable resources and enables a pathway for a decarbonized cleaner chemical industry, for producing green chemicals.

08 HYDROGEN↗

Reevaluation of Radiation-Protection Standards for Workers and the Public Based on Current Scientific Evidence

President Trump’s recent executive orders to “Usher in a Nuclear Renaissance,” coupled with the global pledge to triple nuclear energy capacity by 2050, underscore nuclear energy’s importance to national security and economic prosperity. This renewed interest has prompted efforts to spur nuclear-energy deployment, including assessing factors impeding it. One issue that has previously been identified as adding to the cost of nuclear energy is excessively conservative requirements, including those related to radiation protection. This technical review, therefore, examines current radiation-protection standards that were established decades ago when more limited data were available and nuclear-energy expansion was not a national priority. The review focuses on scientific evidence regarding the health effects of ionizing radiation at annual doses of 10,000 mrem or less. The review evaluates epidemiological studies, radiobiological research, and positions of relevant professional organizations to assess whether such doses result in discernable or observable increases in negative health outcomes. The review also surveys the literature related to economic and practical implications of current radiation-protection standards and practices. Based on this assessment, we propose maintaining an annual occupational whole-body dose limit of 5,000 mrem/yr and eliminating all “as low as reasonably achievable” requirements and limits below this threshold. This change could potentially reduce radiation-protection costs by millions of dollars annually for each reactor, as well as decrease the overall costs and correct misconceptions about the risks associated with all nuclear technologies. The evidence further supports future consideration of a 10,000 mrem/yr limit that would maintain appropriate safety margins while further reducing protection costs. Similarly, given the data and that the average annual radiation dose per person in the U.S. is 620 mrem, we believe the public dose limits of 100 mrem/yr are unnecessarily restrictive; increasing to 500 mrem/yr would maintain substantial safety margins—a factor of 10 below the occupational limit—while reducing regulatory burdens and associated bureaucracy. While we acknowledge ongoing scientific debate and encourage continued research on the health effects of ionizing radiation, our review indicates current frameworks are overly conservative. These overly stringent limits not only impose unnecessary economic burdens without corresponding health benefits but also divert safety focus and resources from more important considerations. Although this study was motivated by nuclear-power considerations, reforms to radiation-protection requirements have significant positive implications for other areas, such as nuclear medical applications, environmental remediation, nuclear-waste management and disposal, and industrial applications of nuclear technologies.

61 RADIATION PROTECTION AND DOSIMETRY↗

Wireless System Development for GaN-Based Transmitters for Advanced Nuclear Reactor Environments

The market for consumer electronics is dominated by Si-based electronics. Many Si-based complementary metal–oxide–semiconductor (CMOS) devices are reaching their limitations in terms of switching frequencies, voltages, currents, and temperatures. Furthermore, these devices are widely known to be susceptible to ionizing radiation and neutrons. Advanced nuclear reactors, especially microreactors and small modular reactors, require wireless electronics that can survive larger neutron and gamma doses than Si CMOS. Because of their size, electronics will need to be placed closer to the reactor cores, and cabling capabilities may be limited. However, GaN high-electron-mobility transistors (HEMTs) have been shown to switch faster with higher gains, and they can achieve current and voltage limits beyond traditional Si CMOS. However, they have less market maturity and have undergone less testing. These GaN HEMTs have been shown to survive ionizing radiation with little effects, but the effects of neutron radiation remain widely unknown. In this report, a wireless electronic system capable of supporting multiple radiation-hardened (rad-hard) sensors is presented. The proposed transmission scheme was designed to be simple to increase the likelihood of success in the immature GaN HEMT process and in high-radiation environments. The transmission system was tested using software-defined radios to emulate the transmission scheme before the transmitter circuitry in the GaN process was developed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Modeling phonon-mediated quasiparticle poisoning in superconducting qubit arrays

Correlated errors caused by ionizing radiation impacting superconducting qubit chips are problematic for quantum error correction. Such impacts generate quasiparticle (QP) excitations in the qubit electrodes, which temporarily reduce qubit coherence significantly. The many energetic phonons produced by a particle impact travel efficiently throughout the device substrate and generate quasiparticles with high probability, thus causing errors on a large fraction of the qubits in an array simultaneously. Here, we describe a comprehensive strategy for the numerical simulation of the phonon and quasiparticle dynamics in the aftermath of an impact. We compare the simulations with experimental measurements of phonon-mediated QP poisoning and demonstrate that our modeling captures the spatial and temporal footprint of the QP poisoning for various configurations of phonon downconversion structures. We thus present a path forward for the operation of superconducting quantum processors in the presence of ionizing radiation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electrochemical Manipulation and Radiolytic Evaluation of Organic Phase Neptunium

Presentation for Seed LDRD proposal presentation: This Seed LDRD research proposes to test an innovative approach to precisely control the oxidation state distribution of neptunium (Np) under used nuclear fuel (UNF) reprocessing conditions using novel electrochemical methods. Current UNF reprocessing technologies are not financially viable in the US, requiring significant scientific and technological innovation to improve cost efficiency. Reducing the number of process cycles is one avenue for increasing cost efficiency, of which resolving the challenge associated with isolating Np is critical. Under envisioned process conditions, Np is present in a mixture of extractable (Np(IV) and Np(VI)) and inextractable (Np(V)) oxidation states, the distribution of which is dependent on several factors, including ionizing radiation dose, that change throughout a reprocessing scheme. Consequently, Np unintentionally partitions into various UNF reprocessing phases and product streams, ultimately increasing the number of process cycles to isolate UNF components. Here, we propose to employ novel, high surface area, optically transparent, Ligand Modified tin-doped indium oxide Electrodes (LMES). These LMEs bind Np, and therefore enable concurrent generation and spectroscopic characterization of Np oxidation states in organic solutions. These proof-of-concept experiments will: (i) facilitate optimization of the proposed electrochemical system conditions for Np oxidation state manipulation; (ii) identify the accessible electrochemical window for Np complexes in the organic phase; (iii) report characteristic optical spectra for each accessible complexed Np oxidation state; and (iv) determine the lifetime and partitioning of a given atypical Np oxidation state in the organic phase in the presence and absence of ionizing radiation fields. The data gathered by this Seed LDRD will provide support for the design of an electrochemical process concept for the precise manipulation of Np oxidation states in UNF reprocessing solvent systems, with the intention of providing advanced control over Np mass transfer, and thus greater process efficiency and economy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Effect of Interleukin-7 on Radiation-Induced Lymphopenia and Its Antitumor Effects in a Mouse Model

Local ionizing radiation (IR) can lead to systemic lymphocyte depletion, which is associated with poor survival outcomes in patients with cancer. Interleukin-7 (IL-7) plays an important role in lymphocyte homeostasis; however, its role in alleviating radiation-induced lymphopenia remains unclear. Hence, we established a radiation-induced lymphopenia animal model and evaluated the effect of exogenous IL-7 administration.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Atomistic‐Level Effects of Noncovalent Interactions and Crystalline Packing for Organic Material Structural Integrity upon Exposure to Gamma Radiation

Developing an atomistic understanding of ionizing radiation induced changes to organic materials is necessary for intentional design of greener and more sustainable materials for radiation shielding and detection. Cocrystals are promising for these purposes, but a detailed understanding of how the specific intermolecular interactions within the lattice upon exposure to radiation affect the structural stability of the organic crystalline material is unknown. This study evaluates atomistic-level effects of γ radiation on both single- and multicomponent organic crystalline materials and how specific noncovalent interactions and packing within the crystalline lattice enhance structural stability. Dose studies were performed on all crystalline systems and evaluated via experimental and computational methods. Changes in crystallinity were evaluated by p-XRD and free radical formation was analyzed via EPR spectroscopy. Type of intermolecular interactions and packing within the crystal lattice was delineated and related to the specific free radical species formed and the structural integrity of each material. Periodic DFT and HOMO-LUMO surface mapping calculations provided atomistic-level identifications of the most probable sites for the radicals formed upon exposure to γ radiation and relate intermolecular interactions and molecular packing within the crystalline lattice to experimental results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗