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At least 55 records · Page 3

In vitro toxicity assessment of uranium particulates on different human lung epithelial cell models

Inhalation of uranium aerosols produced via human activities such as mining can pose a threat to human respiratory systems. Uranium oxide particulates emit short-range alpha particles that elicit DNA and direct damage, beyond associated physiochemical heavy-metal toxicity, to internal epithelial tissues. The availability of reliable in vitro models to study radiation exposure can greatly enhance our ability to understand and combat the biological impacts of exposure. However, the toxicological effects of alpha emissions and/or the oxidation states of uranium particulates vary across different human lung epithelial cell models and have not been systematically compared. We have endeavored to address this limitation by comparing impacts in three different human lung cell models: primary human bronchial and tracheal epithelial cells, primary human small airway epithelial cells, and human adenocarcinoma alveolar basal epithelial cells. Other studies have mainly investigated the toxicity of depleted uranium. Here, we compared the exposure of uranium oxide particulates (U 3 O 8 and UO 3 ) of different enrichment states on the chosen cell systems. Each cell model was exposed to 0.1, 1, 10, 50, 100, and 500 µg/mL of depleted U 3 O 8 , highly-enriched U 3 O 8 , and natural UO 3 particulates for 24 hours in submerged monolayer cultures. We compared viability and superoxide dismutase activity results across cell lines and uranium enrichment/ oxidative states. The results showed that 1) the oxide state of the particulates affected cell viability, implying that uranium’s different oxidation states contribute to different toxicological responses, and 2) each cell model reacts differently when exposed to uranium oxides, which may provide insights into the mechanistic processes associated with the exposure of radiological particulates on different biological systems. For instance, increased uranium enrichment corresponds to increased toxicity for the primary cells, but not for the immortalized cells. Our study shows that a holistic approach that incorporates similarities between model systems and types of radionuclides is required to truly develop empirical solutions for radiation exposure.

59 BASIC BIOLOGICAL SCIENCES↗

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↗

Radiative damping of toroidal Alfvén eigenmode in low-shear plasmas

Instabilities of Alfvén eigenmodes (AEs) are of significant concern because they can enhance the cross-field transport of fusion-born alpha particles beyond the neoclassical level in magnetic fusion plasmas. The threshold value of alpha-particle pressure for exciting AEs depends critically on the damping rate of AEs. The damping mechanisms include kinetic damping due to interactions with thermal particles, continuum damping due to AE frequency crossing Alfvén continuum, and radiative damping due to emitting kinetic Alfvén waves (KAWs). The radiative damping is substantial and can even prevail in high-temperature burning plasmas [1]. We revisit the radiative damping analytic theory for TAE in plasmas with low positive magnetic shear, considering TAE with an eigenfrequency near the bottom of TAE-gap and with poloidal harmonics of the same sign (even TAE). In contrast to earlier papers, we provide the damping calculations in real space rather than Fourier space. This approach is straightforward technically and more enlightening from a physics standpoint for benchmarking numerical calculations of radiative damping. The parametric dependence of the resulting damping rate agrees with that of Refs. [2-5], but it has a smaller numerical factor in front of it.

Alpha-particle driven instability↗

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↗

Device response principles and the impact on energy resolution of epitaxial quantum dot scintillators with monolithic photodetector integration

Abstract Epitaxial quantum dot (QD) scintillator crystals with picosecond-scale timing and high light yield have been created for medical imaging, high energy physics and national security applications. Monolithic photodetector (PD) integration enables the sensing of photons generated within the waveguiding crystal and allows a wide range of scintillator-photodetector coupling geometries. Until recently, these doubly novel devices have suffered from complex, high variance responses to monoenergetic sources which significantly reduces their precision and accuracy. The principles governing the overall device response have now been discerned and embodied by an expression derived within a geometrical optics framework which considers optical properties, surface roughness and photodetector coupling geometry. Response variation due to these factors was sufficiently reduced to obtain material-related energy resolution values of 2.4% with alpha particles. These findings place energy resolution alongside luminescence timescale, photon yield, and radiation hardness as outstanding properties of these engineered materials.

36 MATERIALS SCIENCE↗

Purification Techniques for Actinide Radiolysis Studies

Our fundamental understanding of actinide radiation-induced redox chemistry is crucial due to their unavoidable exposure to ionizing radiation fields, both inherent and from in-process applications. Plutonium (Pu) and americium (Am) both possess multiple oxidation states, the careful manipulation of which are essential in the study and utilization of their rich chemistry, developing new technologies, and securing the long-term sustainability of nuclear power. However, knowledge in this area is far from complete. We have studied the radiation-induced chemistry of both Pu and Am through a variety of techniques, including gamma irradiation, in-situ alpha irradiation and pulse radiolysis experiments. However, for the collection of accurate data, thorough purification and quantification of actinide-containing solutions is required. This presentation will cover the purification and quantification techniques employed for the radiolysis experiments described in our recent publications: Kynman et al., Multiscale Modeling of Plutonium Radiation Chemistry in Nitric Acid Solutions. 1. Cobalt-60 Gamma Irradiation of Pu(IV) [https://pubs.acs.org/doi/10.1021/acs.inorgchem.4c00138] and Kynman et al., Generation and Study of Am(IV) by Temperature-Controlled Electron Pulse Radiolysis [https://doi.org/10.1039/D4DT00991F].

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Alpha-Imaging Detector System Development for Large Area Monitoring

Effective management and disposal of legacy nuclear waste are essential for ensuring safe work environments and minimizing environmental impacts. Monitoring airborne actinide contamination is particularly critical due to the high internal dose potential of alpha-emitting radionuclides. Traditional continuous air monitoring systems (CAMs) used in the industry are limited in the volume of air they can sample, potentially leading to inaccurate radiation detection over large areas. For example, in 2018, elevated levels of airborne Plutonium-239 were detected beyond the controlled areas of the Hanford Plutonium Finishing Plant, highlighting the potential risks to both plant workers and nearby residents. To address these challenges, high-efficiency particulate absorbing (HEPA) air purifiers can enhance air flow by up to 1.5 orders of magnitude, thereby increasing monitoring efficiency and providing a cost-effective solution for large-area surveillance. To quantify the activities of alpha-emitting radionuclides on HEPA filters, the Savannah River National Laboratory is developing an advanced alpha-imaging detection system. This system includes scintillating materials combined with a digital scientific camera. A significant concern in operating such a large-area airborne monitoring system is the handling of HEPA filters, which may be contaminated with radioactive particles. To mitigate these hazards, it is crucial to ensure that any contamination is securely fixed onto the filters. Efforts have been made to optimize the sensitivity of scintillator-epoxy composites and apply them to HEPA filters. These materials were characterized using fluoroscence spectroscopy. These techniques confirmed the purity of the raw materials, the dispersion of scintillators in the epoxy matrix, and the stability of their optical and structural properties post-modification. The optimal scintillator-epoxy composite was selected for use on alpha-spiked HEPA filters to evaluate the efficiency of the sprayer. HEPA filters, embedded with alpha particles collected by an air purifier deployed in an airborne radiation area, have been tested to assess detection efficiency. Future work will focus on employing multiple imaging sensors simultaneously to enhance sensitivity across different regions of the HEPA filter.

Pham, Phuong [Savannah River National Laboratory (↗

SOURCES4D

SOURCES is a code for computing neutron source rates and spectra from spontaneous fission (including delayed neutrons) and (alpha,n) reactions in homogeneous materials and (alpha,n) reactions in single-interface and two-interface geometries. SOURCES is a Los Alamos National Laboratory (LANL) code that is written in FORTRAN and distributed through the Radiation Safety Information Computation Center (RSICC). LANL’s last release of SOURCES to RSICC was SOURCES4C in 2002. This disclosure covers the latest version of SOURCES, SOURCES4D. This version adds sensitivity capabilities for (alpha,n) sources in homogeneous materials. Specifically, SOURCES4D writes new output that can be used to calculate, in post-processing, first and second derivatives of the (alpha,n) source rate density and spectrum with respect to nuclide densities in a homogeneous material and first derivatives of the (alpha,n) source rate density and spectrum with respect to nuclide stopping powers and (alpha,n) cross sections (nuclear data). These derivatives are useful for uncertainty quantification, predictive modeling, and other applications in neutron transport problems.

Favorite, Jeffrey A.↗

The next-generation magnetic recoil spectrometer (MRSnext) on OMEGA and NIF for diagnosing ion temperature, yield, areal density, and alpha heating

The next-generation magnetic recoil spectrometer (MRSnext) is being designed to replace the current MRS at the National Ignition Facility and OMEGA for measurements of the neutron spectrum from an inertial confinement fusion implosion. The MRSnext will provide a far-superior performance and faster data turnaround than the current MRS systems, i.e., a 2× and 6× improvement in energy resolution at the NIF and OMEGA, respectively, and 20× improvement in data turnaround time. The substantially improved performance of the MRSnext is enabled by using electromagnets that provide a short focal plane (12–16 cm) and unprecedented flexibility for a wide range of applications. In addition to being able to measure neutron yield, apparent ion temperature, areal density, and plasma-flow velocity over a wide range of yields, the NIF MRSnext will be able to directly, uniquely assess the alpha heating of the fuel ions through measurements of the alpha knock-on tail in the neutron spectrum. The goal is to implement a radiation-hard electronic detection system capable of providing rapid data acquisition and analysis. The development of the MRSnext will also set the foundation for the more advanced, time-resolving MRSt and serve as a testbed for its implementation on the NIF.

47 OTHER INSTRUMENTATION↗

Sustainable production of radionuclidically pure antimony-119

Background Radiopharmaceutical therapy (RPT) uses radionuclides that decay via one of three therapeutically relevant decay modes (alpha, beta, and internal conversion (IC) / Auger electron (AE) emission) to deliver short range, highly damaging radiation inside of diseased cells, maintaining localized dose distribution and sparing healthy cells. Antimony-119 ( 119 Sb, t 1/2 = 38.19 h, EC = 100%) is one such IC/AE emitting radionuclide, previously limited to in silico computational investigation due to barriers in production, chemical separation, and chelation. A theranostic (therapeutic/diagnostic) pair can be formed with 119 Sb’s radioisotopic imaging analogue 117 Sb (t 1/2 = 2.80 h, E γ = 158.6 keV, I γ = 85.9%, β + = 262.4 keV, I β+ = 1.81%). Results Within, we report techniques for sustainable and cost-effective production of pre-clinical quality and quantity, radionuclidically pure 119 Sb and 117 Sb, novel low energy photon measurement techniques for 119 Sb activity determination, and physical yields for various tin target isotopic enrichments and thicknesses using (p, n) and (d, n) nuclear reactions. Additionally, we present a two-column separation providing a radioantimony yield of 73.1% ± 6.9% (N = 3) and tin separation factor of (6.8 ± 5.5) x 10 5 (N = 3). Apparent molar activity measurements for deuteron produced 117 Sb using the chelator TREN-CAM were measured at 42.4 ± 25 MBq 117 Sb/µmol (1.14 ± 0.68 mCi/µmol), and we recovered enriched 119 Sn target material at a recycling efficiency of 80.2% ± 5.5% (N = 6) with losses of 11.6 mg ± 0.8 mg (N = 6) per production. Conclusion We report significant steps in overcoming barriers in 119 Sb production, chemical isolation and purification, enriched target material recycling, and chelation, helping promote accessibility and application of this promising therapeutic radionuclide. We describe a method for 119 Sb activity measurement using its low energy gamma (23.87 keV), negating the need for attenuation correction. Finally, we report the largest yet-measured 119 Sb production yields using proton and deuteron irradiation of natural and enriched targets and radioisotopic purity > 99.8% at end of purification.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Mortality among workers at the Rocky Flats Plant, 1951–2017

The Rocky Flats (RFs) Plant operated from 1951–1989 as part of the U.S. Department of Energy (DOE) nuclear complex. Its primary mission was weapons component fabrication, whereby workers were potentially exposed to radioactive and non-radioactive hazards. RF worker mortality was compared to the general population, and dose-response relationships between mortality and radiation organ doses were examined. RF workers first employed between 1951 and 1979 for ⩾30 d were identified (n = 9397). Vital status was determined using national and state death records up to 2017. Organ doses from external photons and neutrons irritation and internalised plutonium (Pu), americium (Am), and uranium (U) were modelled as cumulative lagged total doses per year. Beryllium exposure was evaluated as an effect modifier using data from the DOE Nationwide Beryllium Medical Program. Statistical analyses included standardised mortality ratios (SMRs), Cox proportional hazard models, and excess relative risk (ERR) models. Approximately 53.2% of workers were deceased by the end of the study. Nearly 90% were monitored for radiation exposure, with a mean weighted absorbed dose of 59.0 mGy for the lungs. Nearly 45% of workers had intakes of alpha-particle emitting radionuclides, and 46.7% were monitored for neutrons. Leading causes of death included ischemic heart disease (n = 999) and lung cancer (n = 361). The highest SMRs were observed for berylliosis (SMR: 176.9; 95% CI: 76.2, 348.7; n < 10) and asbestosis (SMR: 4.65; 95% CI: 2.23, 8.55; n = 10). Dose-response analyses showed no statistical increase in risk from low-dose radiation including lung cancer (ERR per 100 mGy: −0.02; 95% CI: −0.11, 0.08; n = 361) and Parkinson’s disease (ERR per 100 mGy: 0.13; 95% CI: −0.26, 0.31; n = 57). Approximately 45% of workers were monitored for beryllium, with a weak non-significant indication of effect modification for lung cancer risk. The RF cohort showed no evidence of a statistically significant increase in mortality from occupational radiation exposure. However, this study was limited by low statistical power, which inhibits the ability to detect effects. Future pooling of Million Person Study (MPS) cohorts will provide further insights, particularly regarding Pu as a carcinogen.

61 RADIATION PROTECTION AND DOSIMETRY↗

Field deployable trace radioisotope analysis through combined electrochemical and alpha spectroscopy methods

A method for depositing actinides directly onto a 4H-SiC Schottky barrier diode (SBD) detector as a field deployable actinides sensor was developed to enable off-site analysis, shortening the time to obtain critical information such as elements, concentration, and/or isotopic ratio related to the radiological situation. A thin film of Hg was first electrodeposited onto the Pt contact of the SiC diode, followed by chronoamperometric deposition of microgram levels of actinides under conventional control conditions. The 4H-SiC diode maintained consistent functionality through the electrodeposition process and showed resolved alpha-energy spectra that contained accurate isotopic information demonstrating the feasibility of a combined chemical and radiological sensor for field actinide detection and quantification.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

High-yield implosion modeling using the Frustraum: Assessing and controlling the formation of polar jets and enhancing implosion performance with applied magnetization

Frustraums have a higher laser-to-capsule x-ray radiation coupling efficiency and can accommodate a large capsule, thus potentially generating a higher yield with less laser energy than cylindrical Hohlraums for a given Hohlraum volume [Amendt et al., Phys. Plasmas 26, 082707 (2019]. Frustraums are expected to have less m = 4 azimuthal asymmetries arising from the intrinsic inner-laser-beam geometry on the National Ignition Facility. An experimental campaign at Lawrence Livermore National Laboratory to demonstrate the high-coupling efficiency and radiation symmetry tuning of the Frustraum has been under way since 2021. Simulations benchmarked against experimental data show that implosions using Frustraums can achieve more yield with higher ignition margins than cylindrical Hohlraums using the same laser energy. Hydrodynamic jets in capsules along the Hohlraum axis, driven by radiation-flux asymmetries in a Hohlraum with a gold liner on a depleted uranium (DU) wall, are present around stagnation, and these “polar” jets can cause severe yield degradation. The early-time Legendre mode P4<0 radiation-flux asymmetry is a leading cause of these jets, which can be reduced by using an unlined DU Hohlraum because the shape of the shell is predicted to be more prolate. Magnetization can increase the implosion robustness and reduce the required hotspot ρR for ignition; therefore, magnetizing the Frustraum can maintain the same yield while reducing the required laser energy or increase the yield using the same laser energy—all under the constraint that the ignition margin is preserved. Reducing polar jets is particularly important for magnetized implosions because of the intrinsic toroidal hotspot ion temperature topology.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Toward Rapid Actinium-225 Purification via Membrane Adsorbers with Covalently Tethered Diglycolamide Ligands

Extractive diglycolamide (DGA) resins are used in several state-of-the-art techniques for purifying 225 Ac, a promising radiometal for targeted alpha therapy. Unfortunately, separation processes that rely on resins are often limited to slow flow rates, high elution volumes, and long processing times. Membrane adsorbers functionalized with DGA ligands are an alternative separation material that may overcome these challenges. This work presents (1) the synthesis of an aminated tetrahexyldiglycolamide ligand, (2) the covalent tethering of the ligand to electrospun poly(vinylbenzyl chloride) fiber mats, and (3) the adsorption and desorption of La(III) and 225 Ac. Chemical and physical characterization supports the covalent tethering of the ligand to the fiber mat, as well as the preservation of the fiber surface area and porosity after functionalization. Equilibrium adsorption experiments were performed with stable La(III) and radioactive 225 Ac. Trends in affinity are consistent between commercial resins and the synthesized membrane adsorbers; however, the Langmuir constants and the maximum binding capacity of the membrane adsorbers were generally lower than the resins. Despite these differences, the modeled selectivity for an equimolar solution of La(III)/ 225 Ac in 10 M nitric acid is 57. Furthermore, 225 Ac is rapidly desorbed from the fibers in 10 M nitric acid (<20 min). The La(III)/ 225 Ac selectivity and rapid 225 Ac desorption indicate this class of materials is promising for rapid radioanalytical separations.

07 ISOTOPE AND RADIATION SOURCES↗

Benchmark of the Fe xvv 𝓡 ratio in photoionized plasma during eclipse of Centaurus X-3 with XRISM/Resolve

The $\mathcal {R}$ ratio is a useful diagnostic of the X-ray emitting astrophysical plasmas and is defined as the intensity ratio of the forbidden over the inter-combination lines in the K$\alpha$ line complex of He-like ions. The value is altered by excitation processes (electron impact or UV photoexcitation) from the metastable upper level of the forbidden line, thereby constraining the electron density or UV field intensity. The diagnostic has been applied mostly in electron density constraints in collisionally ionized plasmas using low-Z elements, as was originally proposed for the Sun (Gabriel & Jordan, 1969a, MNRAS, 145, 241), but it can also be used in photoionized plasmas. To make use of this diagnostic, we need to know its value in the limit of no excitation of metastables ($\mathcal {R}_{0}$), which depends on the element, how the plasmas are formed, how the lines are propagated, and the spectral resolution affecting line blending principally with satellite lines from Li-like ions. We benchmark $\mathcal {R}_0$ for photoionized plasmas by comparing calculations using radiative transfer codes and observation data taken with the Resolve X-ray microcalorimeter onboard XRISM. We use the Fe xxv He$\alpha$ line complex of the photo-ionized plasma in Centaurus X-3 observed during eclipse, in which the plasma is expected to be in the limit of no metastable excitation. The measured $\mathcal {R} = 0.65 \pm 0.08$ is consistent with the value calculated using xstar for the plasma parameters derived from other line ratios of the spectrum. We conclude that the $\mathcal {R}$ ratio diagnostic can be used for high-Z elements such as Fe in photoionized plasmas, which has wide applications in plasmas around compact objects at various scales.

X-rays: binaries↗

Active tungsten expulsion in ELM-absent H-mode plasmas via on-demand ELM triggering with lithium granule injection

Lithium granules gravitationally injected into the upper X-point region demonstrated on-demand edge-localized modes (ELM) triggering in otherwise ELM-suppressed H-mode plasmas on the Experimental Advanced Superconducting Tokamak. Sub-mm lithium granules dropped into enhanced D-alpha H-mode plasmas achieved a high triggering efficiency, while enabling ELM frequencies from several to hundreds of hertz. Core radiation from heavy impurities, dominated by W, was reduced by up to 60%, and the normalized energy confinement increased by up to 30%. At low injection frequencies, ELMs of substantially reduced size compared to spontaneous type-I ELMs were observed. At high injection frequencies, a transition to a mixed ELM phase occurred, characterized by intermittent larger ELMs and suppression of the quasi-coherent mode, achieving the most significant W reduction and energy confinement improvement. These results highlight a promising pathway for active W control via controlled, small ELMs in long-pulse, high-performance scenarios.

EDA H-mode↗

Measurement of the Ground State Spin and Parity of 22 Al Disfavors Halo Formation

We report the decisive resolution of the ground state spin and parity of the proton–drip line nucleus 22 Al, a prime candidate for a proton halo. The resolution stems from the first 𝛽-delayed charged particle emission experiment in the gas stopping area at the Facility for Rare Isotope Beams (FRIB), leveraging high-intensity, low-energy beams extracted from the Advanced Cryogenic Gas Stopper (ACGS). The pristine beam quality from FRIB and the ACGS enabled a sensitive particle identification technique using thin silicon detectors, allowing for the suppression of the dominant proton background and the first observation of the weak 𝛽-delayed 𝛼 transition from the isobaric analog state in 22 Mg to the 18 Ne ground state. This observation uniquely fixes the 22 Al ground state as 4 + . The valence proton is confined by a dominant 𝑑-wave centrifugal barrier which, combined with the Coulomb repulsion, hinders the tunneling required for halo formation despite the exceptionally low proton separation energy of 22 Al.

20 ≤ A ≤ 38↗