Spatially Localized Immunotherapy: A Perfect Combination With Radiation Therapy?
No abstract prepared.
62 RADIOLOGY AND NUCLEAR MEDICINE↗
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Best Practices for Shielding Analyses of Activated Metals and Spent Resins from Reactor Operation
This report investigated best practices for performing shielding evaluations of Type B waste packages, as defined in 10 CFR Part 71 regulations on packaging and transportation of radioactive material, or packages for which the contents are not defined before loading and may include a broad range of nuclides, geometries, and non-fuel materials. The following non-fuel waste streams were analyzed: Activated metals from decommissioned commercial power reactors, including Type 304 stainless steel, reactor vessel steel, and Inconel, Control blades from boiling water reactors, Neutron-activated corrosion products on surfaces of activated metals, and Spent resins from power plant operations. Measured elemental compositions, including major constituents and impurities, for steel and Inconel samples from commercial power reactors were used in activation calculations to determine radionuclide inventories in activated metals. For a simplified cask model, 60 Co contribution to the total external package dose rate at 30 days after shutdown varied from approximately 60% to 95%, depending on the activated metal, initial cobalt impurity concentration in the metal, and the thickness of the overpack gamma shield. Its maximum contribution to the total external package dose rate of approximately 100% was reached within the time interval of 2 to 5 years after shutdown and was maintained for up to 45 to 60 years after shutdown, depending on material, initial cobalt impurity concentration, and shield thickness. Thereafter, the 60 Co contribution to external package dose rate decreased with increasing decay time. Cobalt-60 is primarily produced by neutron reactions with the cobalt impurity in steel and Inconel. Other important radionuclides in activated metals contributing to package external dose rate are radionuclides with relatively short decay times, including 51 Cr, 59 Fe, 58 Co, and 54 Mn. These radionuclides may be represented as an equivalent 60 Co activity/source because 60 Co gamma ray emissions are bounding in terms of source strength and energy to other important radionuclides identified in the analyzed activated metals. Approaches for modeling the neutron-activated corrosion products that may be attached to activated reactor components were analyzed in this report. It was demonstrated that a surface source is more conservative than a uniform volumetric source for the treatment of neutron-activated corrosion products with respect to external package dose rates. An analysis of the maximum radionuclide loadings reported on spent resins identified the radionuclides 137 Cs, 60 Co, 134 Cs, 65 Zn, and 58 Co as the primary contributors to external package dose rate. For a resin cooled for 3.08 years, the external package dose rate was entirely produced by the reported 137 Cs and 60 Co inventory. The neutron sources from actinides found on spent resins or activated metals produced negligible dose rates and may be ignored in dose rate analyses. Effects of idealized waste material, source geometry, and spatial material/source distributions on external package dose rates were determined based on dose rate results for a simplified cask model under normal conditions of transport. Type 304 stainless steel, zirconium, and aluminum with adjusted mass densities based on a maximum content weight were analyzed for material modeling effects on external package dose rate. These materials produced identical external package dose rates within the statistical uncertainties of the dose rate estimates. Among four different source geometry configurations with homogeneous material of different mass densities, uniform volumetric source distribution, and the same source strength, the geometry configuration with lowest mass density (i.e., minimum self-shielding effect among the four cases) was most conservative. Spatial source distributions that better represent localized peak 60 Co activity values were more conservative than a uniform volumetric source distribution, assuming the same weight and total source strength per package. The increase in external dose rate caused by localized source peaks can be as much as the ratio between source peak activity density to average activity density, depending on the location of the activated metal with peak activity density. Therefore, the shielding analysis may be simplified if localized peak activities and the average activity per package can be measured/determined and documented at the time of cask loading. For simplicity, external package dose rates may be determined based on average source activity and a uniform volumetric source distribution. The dose rate results from that calculation model multiplied by the ratio of peak activity density to average activity density will produce maximum dose rate values for conservative estimates.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Status of the MARS code
This report describes major features of the most recent version of the MARS code as well as ongoing developments. The list of features includes various options for geometry models, a beam line builder based on MADX code, import of geometry models in GDML format, use of structured and unstructured meshes for scoring purposes, an update to the recent TENDL library for a number of projectiles at low energies (up to 250 MeV), and a recently implemented method to calculate spatial distribution of residual dose in a single computer run without an intermediate source. Examples of the code application to various projects are presented as well.
Rakhno, Igor [Fermilab] (ORCID:0000000265828058)↗
A data science approach for analysis and reconstruction of spinodal-like composition fields in irradiated FeCrAl alloys
A statistical method for the analysis of continuously distributed data representative of composition fluctuations in irradiated FeCrAl alloys acquired using Energy Dispersive X-ray Spectroscopy (EDS) method is presented. Using probability distribution functions, direct and cross-covariances between the elemental compositions, the effects of alloy composition and irradiation dose were investigated on the spatial distribution and length scale of composition fluctuations at the nanoscale. We have observed that, for neutron-irradiated FeCrAl alloys, the distribution of Fe and Cr followed a left-skewed and right-skewed distribution, respectively for all (average) alloy compositions and irradiation doses. The analysis also revealed enhanced spatial gradients in the elemental compositions at higher irradiation dose. Direct and cross-covariance estimates of the experimental data were also utilized for reconstruction of composition data through fitting it to a parametric form of the covariance functions. Linear Model of Coregionalization was used to determine the parameters of the covariance functions. Subsequently, a spectral method was utilized for simulating a realization of the alloy compositions. Close correspondence was observed between the experimental and the reconstructed data which was analyzed using probability distribution functions and covariance functions. Composition space of the experimental and reconstructed data and dislocation velocities as a function of applied stress and line directions over the entire composition maps were also examined.
36 MATERIALS SCIENCE↗
Sources of Conservatism in Making Corrective Action Decisions at the NNSS - 20477
During the course of closing nuclear testing release sites at the Nevada National Security Site (NNSS) under the Federal Facility Agreement and Consent Order (FFACO) using the Risk-Based Corrective Action (RBCA) evaluation process, conservative assumptions and estimates were used in many phases of the work. These assumptions and estimates were agreed to during Data Quality Objective (DQO) meetings and published in the FFACO documents. However, the potential cumulative effect of these multiple sources of conservatism was not evaluated. The RBCA process ensures that corrective action decisions minimize the risk of making Type I errors (not applying corrective action to areas that exceed action levels) at the expense of making Type II errors (applying corrective action to areas that do not exceed action levels). Rather than fully characterizing the spatial distribution of contaminants throughout each site, the RBCA process uses a bounding methodology that conservatively estimates spatial boundaries beyond which contamination is not present that exceed corrective action levels. This process accepts that these boundaries may encompass areas that do not exceed corrective action levels and, therefore, may be somewhat larger than for fully characterized sites. This is justified at sites where the reduction in investigation costs are more than any potential increase in corrective action costs. To minimize the risk of making Type I errors, conservatism was used throughout the process. This study documents the many sources of conservatism used in the RBCA process. Conservatism was used in the RBCA process in determining potential receptors, determining action levels, collecting samples, converting sample results into receptor dose, and accounting for uncertainty. This provides decision-makers with a high level of confidence that unacceptable risk to receptors will not result from exposure to residual contamination outside the corrective action boundaries. However, it does not provide an estimate of the actual extent of areas exceeding action levels. This study provides an evaluation of the effects of compounding conservatism on RBCA process decisions. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Monte Carlo Simulations in Support of NorthStar Irradiation Facility Commissioning Procedure
NorthStar Medical Radioisotopes LLC is constructing an irradiation facility at which electron accelerators will induce photo-transmutation (i.e., neutron knockout) of molybdenum-100 (Mo-100) to produce medically useful Mo-99. The facility will house two high-intensity electron RhodotronTM accelerators developed by IBA Industrial. The nominal power of each Rhodotron is 125kW at 40 MeV beam energy. The production target is made of metallic molybdenum enriched with Mo-100 isotope. It will be irradiated by electron beams and will itself play a role in electron conversion to intense X-rays. A full description of the NorthStar target as well as the concept of radiation shielding of the facility can be found in our previous report. The NorthStar irradiation facility is under commissioning now. The goal of the present work is to support the commissioning process by: (1) Studying residual radiation and activation to minimize personnel exposure and inform radiation waste management; (2) Using computational fluid dynamics (CFD) of the irradiated target to ensure the facility design is safe and reliable; and (3) Helping to determine radiation protection requirements during operation. Monte Carlo simulations are used for the analyses. Most of the results are presented as 3D arrays representing spatial distribution of values across simulated geometries: radiation energy depositions, ambient doses, residual isotopes accumulated, and residual doses.
07 ISOTOPE AND RADIATION SOURCES↗
Intrinsic Li Distribution in Layered Transition-Metal Oxides Using Low-Dose Scanning Transmission Electron Microscopy and Spectroscopy
Understanding Li distribution in layered lithium transition-metal oxide (LiTMO) cathodes in Li-ion batteries has been a major challenge at the atomic scale and nanoscale. Li is extremely difficult to study by transmission electron microscopy (TEM) because the high-energy electrons impart significant energy and cause massive migration. Here, we directly map the intrinsic spatial distribution and bonding of Li in LiNiO 2 -layered cathode materials using low-dose and low-loss electron energy loss spectroscopy (EELS). EELS spectra of the Li–K edge are measured simultaneously with O–K and Ni–L, M 3,2 edges from layered, cation-mixed, and rock-salt phases and directly matched with atomic-resolution scanning TEM images to correlate the changes in peak intensities and positions to the stoichiometry changes with continual loss of Li and O. Changes in the Li content in the LiNiO 2 particles as a function of electron beam dose are studied by sequential Li spectroscopic mapping. We show that the “intrinsic” Li distribution can be observed using a total dose of less than ~1.5 × 10 8 e – nm –2 at an accelerating voltage of 80 kV. The method of nanoscale mapping of Li distribution introduced in this study is applicable to high-Ni LiTMO cathode materials (>89% of Ni) as well as LiNiO 2 . Further study on the extra peaks of the Li–K edge reveals that the peak at ~59 eV is from the Li ions intercalated in between NiO 2 layers barely interacting with each other with less Li K shell electrons pulled to the L shell electrons in NiO 2 . Furthermore, the results shown here provide improved low-loss TEM characterization approaches that can be used to understand the intrinsic fundamental behaviors in Li-ion batteries.
25 ENERGY STORAGE↗
Spatial and temporal prediction of radiation dose rates near Fukushima Daiichi Nuclear Power Plant
In this paper, we have developed a methodology to estimate the spatiotemporal distribution of radiation air dose rates around the Fukushima Daiichi Nuclear Power Plant (FDNPP). In our exploratory data analysis, we found that (1) the temporal evolution of dose rates is composed of a log-linear decay trend and fluctuations of air dose rates that are spatially correlated among adjacent monitoring posts; and (2) the slope of the log-linear environmental decay trend can be represented as a function of the apparent initial dose rates, coordinate position, land-use type, and soil type. From these observations, we first estimated the log-linear decay trend at each location based on these predictors, using the random forest method. We then developed a modified Kalman filter coupled with a Gaussian process model to estimate the dose-rate time series at a given location and time. We applied this method to the Fukushima evacuation zone (as of March 2017), which included 17 monitoring post locations (with monitoring datasets collected between 2014 and 2018) and generated a time series of dose-rate maps. Our results show that this approach allows us to produce accurate spatial and temporal predictions of radiation dose-rate maps using limited spatiotemporal measurements.
61 RADIATION PROTECTION AND DOSIMETRY↗
Kinetic Monte Carlo simulations of aging in δ -Pu
We have developed a first-passage kinetic Monte Carlo approach for materials aging to investigate the sensitivity of void swelling to model parameters, including helium bubble density and size distribution. In addition to explicitly accounting for the spatial distribution of individual point defects, bubbles, and voids, our approach can simulate total doses equivalent to 100 years of natural aging on statistically representative volumes of materials. This technique enables us to study the effects on swelling and radiation damage evolution due to temperature and dose rate (as altered in artificially aged experiments), differences in effective interaction radii between vacancies and interstitials, and varying defect diffusion activation energies, while providing more detailed information than previous rate-equation based approaches. In conclusion, our results indicate that spatial effects that are not modeled in mean-field rate theories could play a significant role in void swelling initiation and growth for certain regimes of model parameters.
Actinides↗
Microstructure-Dependent Rate Theory Model of Radiation-Induced Segregation in Binary Alloys
Conventional rate theory often uses the mean field concept to describe the effect of inhomogeneous microstructures on the evolution of radiation induced defect and solute/fission product segregation. However, the spatial and temporal evolution of defects and solutes determines the formation and spatial distribution of radiation-induced second phase such as precipitates and gas bubbles/voids, especially in materials with complicated microstructures and subject to high dose radiation. In this work, a microstructure-dependent model of radiation-induced segregation (RIS) has been developed to investigate the effect of inhomogeneous thermodynamic and kinetics properties of defects on diffusion and accumulations of solute A in AB binary alloys. Four independent concentrations: atom A, interstitial A, interstitial B, and vacancy on [A, B] sublattice are used as field variables to describe temporal and spatial distribution and evolution of defects and solute A. The independent concentrations of interstitial A and interstitial B allow to describe their different generation rates, thermodynamic and kinetic properties, and release the assumptions of interstitial generation and sink strength used in the conventional rate theory. Microstructure and concentration dependent chemical potentials of defects are used to calculate the driving forces of defect diffusions. With the model, the effects of defect chemical potentials and mobilities on the RIS in polycrystalline AB model alloys have been simulated. The results demonstrated the model capability in predicting defect evolution in materials with inhomogeneous thermodynamic and kinetic properties of defects. The model can be extended to materials with complicated microstructures such as a wide range of grain size distribution, coating structure and multiphases as well as radiation-induced precipitation subject to severe radiation damage.
36 MATERIALS SCIENCE↗
Ionization detail parameters and cluster dose: a mathematical model for selection of nanodosimetric quantities for use in treatment planning in charged particle radiotherapy
Abstract Objective . To propose a mathematical model for applying ionization detail (ID), the detailed spatial distribution of ionization along a particle track, to proton and ion beam radiotherapy treatment planning (RTP). Approach . Our model provides for selection of preferred ID parameters ( I p ) for RTP, that associate closest to biological effects. Cluster dose is proposed to bridge the large gap between nanoscopic I p and macroscopic RTP. Selection of I p is demonstrated using published cell survival measurements for protons through argon, comparing results for nineteen I p : N k , k = 2, 3, …, 10, the number of ionizations in clusters of k or more per particle, and F k , k = 1, 2, …, 10, the number of clusters of k or more per particle. We then describe application of the model to ID-based RTP and propose a path to clinical translation. Main results . The preferred I p were N 4 and F 5 for aerobic cells, N 5 and F 7 for hypoxic cells. Significant differences were found in cell survival for beams having the same LET or the preferred N k . Conversely, there was no significant difference for F 5 for aerobic cells and F 7 for hypoxic cells, regardless of ion beam atomic number or energy. Further, cells irradiated with the same cluster dose for these I p had the same cell survival. Based on these preliminary results and other compelling results in nanodosimetry, it is reasonable to assert that I p exist that are more closely associated with biological effects than current LET-based approaches and microdosimetric RBE-based models used in particle RTP. However, more biological variables such as cell line and cycle phase, as well as ion beam pulse structure and rate still need investigation. Significance . Our model provides a practical means to select preferred I p from radiobiological data, and to convert I p to the macroscopic cluster dose for particle RTP.
Engineering↗
Particle showers detected on ISS in Timepix pixel detectors
We detect regular particle showers in several compact pixel detectors, distributed over the International Space Station. These showers are caused by high energy galactic cosmic rays, with energies often in the 10 s of TeV or higher. We survey the frequency of these events, their dependence on location on ISS, and their independence of the location of ISS, on its orbit. The Timepix detectors used allow individual particle tracks to be resolved, providing a possibility to perform physical analysis of shower events, which we demonstrate. In terms of radiation dosimetry, these showers indicate certain possible limitations of traditional dosimetric measures, in that (a) the dose measured in small sensor may be less than that received in a larger distribution of matter, such as a human and (b) the spatial and temporal extent of these events represents a regime of poorly documented biological response.
79 ASTRONOMY AND ASTROPHYSICS↗
Highly Tunable Thiol-Ene Photoresins for Volumetric Additive Manufacturing
Volumetric additive manufacturing (VAM) forms complete 3D objects in a single photocuring operation without layering defects, enabling 3D printed polymer parts with mechanical properties similar to their bulk material counterparts. This study presents the first report of VAM-printed thiol-ene resins. With well-ordered molecular networks, thiol-ene chemistry accesses polymer materials with a wide range of mechanical properties, moving VAM beyond the limitations of commonly used acrylate formulations. Since free-radical thiol-ene polymerization is not inhibited by oxygen, the nonlinear threshold response required in VAM is introduced by incorporating 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO) as a radical scavenger. Tuning of the reaction kinetics is accomplished by balancing inhibitor and initiator content. Coupling this with quantitative measurements of the absorbed volumetric optical dose allows control of polymer conversion and gelation during printing. Importantly, this work thereby establishes the first comprehensive framework for spatial–temporal control over volumetric energy distribution, demonstrating structures 3D printed in thiol-ene resin by means of tomographic volumetric VAM. Mechanical characterization of this thiol-ene system, with varied ratios of isocyanurate and triethylene glycol monomers, reveals highly tunable mechanical response far more versatile than identical acrylate-based resins. This broadens the range of materials and properties available for VAM, taking another step toward high-performance printed polymers.
36 MATERIALS SCIENCE↗
Correlation of Processing and Structure in an Ethylene‐Glycol Side‐Chain Modified Polythiophene via Combined X‐Ray Scattering and 4D Scanning Transmission Electron Microscopy
The results of a combined grazing incidence wide-angle X-ray scattering (GIWAXS) and 4D scanning transmission microscopy (4D-STEM) analysis of the effects of thermal processing on poly(3[2-(2-methoxyethoxy)ethoxy]-methylthiophene-2,5-diyl) are reported, a conjugated semiconducting polymer used as the active layer in organic electrochemical transistor devices. GIWAXS provides a measure of overall crystallinity in the film, while 4D-STEM produces real-space maps of the morphology and orientation of individual crystallites along with their spatial extent and distribution. The sensitivity of the 4D-STEM detector allows for collection of electron diffraction patterns at each position in an image scan while limiting the imparted electron dose to below the damage threshold. In conclusion, the effects of heat treatment on the distribution and type of crystallites present in the films is determined.
36 MATERIALS SCIENCE↗
Surprisingly high irradiation-induced defect mobility in Fe 3 O 4 as revealed through in situ transmission electron microscopy
Radiation-induced defects are expected to change the corrosion kinetics when a material is exposed to a corrosive environment. Characterization of the defects forming under irradiation and their ability to move/diffuse is therefore key to understanding how they impact the corrosion kinetics and possibly mechanisms. For that matter, Fe/Fe 3 O 4 interfaces were irradiated using 1 MeV Kr 2+ at temperatures of 273 K (25 °C), 573 K (300 °C) and 773 K (500 °C) to a maximum dose of 10 dpa (as measured in the Fe matrix) in situ in a transmission electron microscope. The evolution of the microstructure was followed as a function of the dose and temperature. The formation of defects was followed in the metal and the oxide as well as at the metal/oxide interface and characterized in terms of size and density. Additionally, the dynamic observation of the spatial distribution of the defects allowed for a qualitative assessment of the mobility of defects in the oxide as a function of temperature, revealing evidence for enhanced mobility even more so than in the Fe matrix. Mechanisms of induced defect mobility in the spinel are discussed to account for the observations.
36 MATERIALS SCIENCE↗
An effective QWBA/UHPLC-MS/tissue punch approach: solving a pharmacokinetic issue via quantitative Met-ID
Methods to provide absolute quantitation of the administered drug and corresponding metabolites in tissue in a spatially resolved manner is a challenging but much needed necessity in pharmaceutical research. Quantitative whole-body autoradiography (QWBA) after a single-dose intravenous (3 mg/kg) and extravascular (30 mg/kg) administrations of an in vitro metabolically stable test compound (structure not reported here) indicated quick tissue distribution and excretion. Good bioavailability and short in vivo half-lives were determined formerly for the same test compound. For closing gaps in the understanding of pharmacokinetic data and in vitro results, radioactive hot spots on whole-body tissue sections had been profiled. Punches from selected tissue regions containing high radioactivity in the tissue sections previously analyzed by QWBA were extracted by a highly organic solvent and analyzed without any consecutive sample preparation step, applying ultra high performance liquid chromatography-mass spectrometry (UHPLC-MS) and off-line radioanalysis to maximize signal levels for metabolite identification and profiling. The analysis revealed that the test compound was metabolized intensively by phase I reactions in vivo and the metabolites formed were excreted in bile and in urine. The predominant metabolites showed abundant signal intensities both by MS and by radioanalysis but the MS signal intensities generally underestimated the real abundances of metabolites relative to the unchanged drug. In this work we illustrate that maximizing the sensitivity of tissue punch radioanalysis and the combination with UHPLC-MS leads to a better insight of pharmacokinetic processes by providing quantitative data with high molecular selectivity.
60 APPLIED LIFE SCIENCES↗
The impact of sampling scale: A comparison of methods for estimating external contaminant exposure in free-ranging wildlife
The impacts of contaminants on wildlife are dose dependent, and thus being able to track or predict exposure following contamination events is important for monitoring ecosystem health. However, the ability to track exposure in free-ranging wildlife is often severely limited. Consequently, researchers have predominantly relied on simple methods for estimating contaminant exposures in wildlife with little regard for spatial contaminant heterogeneity or an animal’s use of diverse habitats. We evaluated the influence sampling scale (i.e., how finely contaminant distribution and organism’s spatial use of the landscape is mapped) has on (1) realism and (2) conservativeness of exposure estimates. To do this, we monitored the actual exposure of wild boar (Sus scrofa) in Fukushima, Japan to radioactive contamination using GPS27 coupled contaminant monitors placed on individual animals. We compared empirical exposures to estimates generated by combining varying amounts of information about an individual boar’s location and/or movement, with the distribution of contamination on the landscape. Here we found that the most realistic exposure estimates were produced when finer-scale contaminant distribution surveys (e.g., airborne surveys) were combined with more accurate estimates of an individual’s space use (e.g., home ranges or core areas). Importantly, estimates of exposure based on single point surveys at a trap site (a simple method commonly used in the literature), did not correlate with actual exposure rates, suggesting dose-effects studies using this method may result in spurious conclusions. These results suggest that researchers seeking realistic estimates of exposure, such as in dose-effect studies, should ensure they have adequately accounted for fine-scale contaminant distribution patterns and areas of higher use by study organisms. However, conservative estimates of exposure i.e., intentionally over-predicting exposure as is done in initial tiers of ecological risk analyses) were not as scale sensitive and could be achieved with a single known location and coarse contaminant distribution maps.
63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
Focused Helium Ion Beam for Direct Patterning of Monolayer MoS 2 Nanoribbon Field Effect Devices
The helium ion microscope (HIM) focused ion beam (FIB) has emerged as a powerful tool to directly pattern nanostructures below 10 nm due to its high-resolution capabilities and the inert nature of the ion source. These attributes make HIM FIB particularly interesting for patterning 2D materials such as transition metal dichalcogenides (TMDs) to investigate transport phenomena at the nanoscale. Reported here is the fabrication of MoS 2 nanoribbon devices using HIM FIB-induced etching (FIBIE) with XeF 2 , allowing for reduced ion dose compared to direct sputtering. While patterning is efficacious, the devices exhibit performance degradation with decreasing nanoribbon width due to damage up to 150 nm beyond the patterned edge. Incorporating an hBN encapsulation improves device performance by one order of magnitude, although the lateral extent of damage remains unchanged. The spatial distribution of damage is shown to be determined by the forward- and backscattered ions and electrons, while the hBN encapsulation layer substantially reduces damage from XeF 2 interactions in unexposed regions. Raman and photoluminescence (PL) measurements corroborate these findings, while ion/solid interaction simulations further elucidate the resolution limits imposed by substrate interactions. In conclusion, this work provides critical insights and a practical pathway for utilizing HIM FIBIE in 2D TMD functional device patterning.
MoS 2↗