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DOE OSTI2021

Determination of X-ray detection limit and applications in perovskite X-ray detectors

X-ray detection limit and sensitivity are important figure of merits for perovskite X-ray detectors, but literatures lack a valid mathematic expression for determining the lower limit of detection for a perovskite X-ray detector. In this work, we present a thorough analysis and new method for X-ray detection limit determination based on a statistical model that correlates the dark current and the X-ray induced photocurrent with the detection limit. The detection limit can be calculated through the measurement of dark current and sensitivity with an easy-to-follow practice. Alternatively, the detection limit may also be obtained by the measurement of dark current and photocurrent when repeatedly lowering the X-ray dose rate. While the material quality is critical, we show that the device architecture and working mode also have a significant influence on the sensitivity and the detection limit. Our work establishes a fair comparison metrics for material and detector development.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Sample spinning to mitigate polarization artifact and interstitial-vacancy imbalance in ion-beam irradiation

Accelerator-based ion-beam irradiation has been widely used to mimic the effects of neutron radiation damage in nuclear reactors. However, ion radiation is most often monodisperse in the incoming ions’ momentum direction, leading to excessive polarization in defect distribution, while the scattering under neutron irradiation is often more isotropic and has less radiation-induced polarization. Mitigation of the excess-polarization as well as the damage non-uniformity artifact might be crucial for making the simulation of neutron radiation by ion-beam radiation more realistic. In this work, a general radiation polarization theory in treating radiation as external polar stimuli is established to understand the natural material responses in different contexts, and the possibility to correct the defect polarization artifact in ion-beam irradiation. Inspired by Magic Angle Spinning in Nuclear Magnetic Resonance, we present a precise sample spinning strategy to reduce the point-defect imbalance effect in ion-beam irradiation. It can be seen that with optimized surface inclination angle and the axis of sample rotation, the vacancy-interstitial population imbalance, as well as the damage profile non-uniformity in a designated region in the target are both reduced. It is estimated that sample spinning frequency on the order of kHz should be sufficient to scramble the ion momentum monodispersity for commonly taken ion fluxes and dose rates, which is experimentally feasible.

36 MATERIALS SCIENCE↗

DOE OSTI2023

A new approach for simulating inhomogeneous chemical kinetics

Abstract In this paper, inhomogeneous chemical kinetics are simulated by describing the concentrations of interacting chemical species by a linear expansion of basis functions in such a manner that the coupled reaction and diffusion processes are propagated through time efficiently by tailor-made numerical methods. The approach is illustrated through modelling $$\alpha$$ α - and $$\gamma$$ γ -radiolysis in thin layers of water and at their solid interfaces from the start of the chemical phase until equilibrium was established. The method’s efficiency is such that hundreds of such systems can be modelled in a few hours using a single core of a typical laptop, allowing the investigation of the effects of the underlying parameter space. Illustrative calculations showing the effects of changing dose-rate and water-layer thickness are presented. Other simulations are presented which show the approach’s capability to solve problems with spherical symmetry (an approximation to an isolated radiolytic spur), where the hollowing out of an initial Gaussian distribution is observed, in line with previous calculations. These illustrative simulations show the generality and the computational efficiency of this approach to solving reaction-diffusion problems. Furthermore, these example simulations illustrate the method’s suitability for simulating solid-fluid interfaces, which have received a lot of experimental attention in contrast to the lack of computational studies.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2022

Characterization of self-magnetic pinch (SMP) radiographic diode performance on RITS-6 at Sandia National Laboratories. I. Diode dynamics, DC heating to extend radiation pulse

Radiographic diodes focus on an intense electron beam to a small spot size to minimize the source area of energetic photons for radiographic interrogation. The self-magnetic pinch (SMP) diode has been developed as such a source and operated as a load for the six-cavity radiographic integrated test stand (RITS-6) inductive voltage adder driver. While experiments support the generally accepted conclusion that a 1:1 aspect diode (cathode diameter equals anode–cathode gap) delivers optimum SMP performance, such experiments also show that reducing the cathode diameter, while reducing spot size, also results in reduced radiation dose, by as much as 50%, and degraded shot reproducibility. Analysis of the effective electron impingement angle on the anode converter with time made possible by a newly developed dose-rate array diagnostic indicates that fast-developing oscillations of the angle are correlated with early termination of the radiation pulse on many of the smaller-diameter SMP shots. This behavior as a function of relative cathode size persists through experiments with output voltages and currents up to 11.5 MV and 225 kA, respectively, and with spot sizes below approximately few millimeters. Since simulations to date have not predicted such oscillatory behavior, considerable discussion of the angle behavior of SMP shots is made to lend credence to the inference. We report there is clear anecdotal evidence that DC heating of the SMP diode region leads to stabilization of this oscillatory behavior. This is the first of two papers on the performance of the SMP diode on the RITS-6 accelerator.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

In situ measurements of non-equilibrium positron state defects during He irradiation in Si

Radiation-induced property changes in materials originate from the energy transfer from an incoming particle to the existing lattice, displacing atoms. The displaced atoms can cause the formation of extended defects including dislocation loops, voids, or precipitates. The non-equilibrium defects created during damage events determine the extent of these larger defects and are a function of dose rate, material, and temperature. However, these defects are transient and can only be probed indirectly. Herein, we present direct experimental measurements and evidence of irradiated non-equilibrium vacancy formation, where in situ positron annihilation spectroscopy was used to prove the generation of non-equilibrium defects in silicon.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Design of a high-temperature cell for cobalt-60 irradiations of aqueous solutions with in situ UV–visible spectroscopy

To understand the speciation of solutes in aqueous solutions in high temperature radiation environments, we report the design and fabrication of a custom-built, high temperature (≤300 °C) titanium irradiation cell with in situ optical spectroscopy capabilities, as afforded by coupled fiber optic cables. The wetted surfaces of the 8-inch tall cylindrical cell with 3.5 in. diameter are entirely made of titanium, sapphire, and gold, which are chemically and radiolytically inert. The initial benchmarking results are reported, including the baseline spectrum of deionized water as a function of temperature, the stability of a spectrum over 4 h at 100 °C, and an irradiated Fricke dosimetry solution under ambient irradiator temperature conditions (27.0 ± 0.5 °C). Further, the average gamma radiation dose rate in the cell in its current configuration is 26.1 ± 1.3 Gy min -1 . This cell has application in studying several processes throughout the nuclear fuel cycle, including the reactor coolant behavior.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2023

Machine Learning Surrogates of a Fuel Matrix Degradation Process Model for Performance Assessment of a Nuclear Waste Repository

Spent nuclear fuel repository simulations are currently not able to incorporate detailed fuel matrix degradation (FMD) process models due to their computational cost, especially when large numbers of waste packages breach. The current paper uses machine learning to develop artificial neural network and k-nearest neighbor regression surrogate models that approximate the detailed FMD process model while being computationally much faster to evaluate. Further, using fuel cask temperature, dose rate, and the environmental concentrations of CO 3 2- , O 2 , Fe 2+ , and H 2 as inputs, these surrogates show good agreement with the FMD process model predictions of the UO 2 degradation rate for conditions within the range of the training data. A demonstration in a full-scale shale repository reference case simulation shows that the incorporation of the surrogate models captures local and temporal environmental effects on fuel degradation rates while retaining good computational efficiency.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Decay Dose Shielding Analysis with Hybrid Unstructured Mesh/Constructive Solid Geometry Monte Carlo Calculation and ADVANTG Acceleration

Here, the target segments of the Oak Ridge National Laboratory Second Target Station (STS) neutron production facility become highly activated due to spallation reactions or nuclei transmutation by primary protons and emitted neutrons. Once the target segments are removed from their location within the core vessel, decay dose rates must be accurately quantified to determine the shielding configurations of remote-handling tools and transport casks and to aid in planning maintenance activities. For this analysis, we utilized a hybrid unstructured mesh (UM)/constructive solid geometry approach for calculating spallation products and neutron fluxes, activation calculations using the AARE package that includes the CINDER2008 activation code to calculate the decay photon source at different cooling times, and the ADVANTG code to accelerate the final decay photon transport calculation. Both Type 316 stainless steel (SS-316) and lead were investigated as candidates for shielding materials. The decay photon transport calculation through the thick SS-316 or lead shields exhibited between 25 and 30 orders-of-magnitude attenuations in the radial direction, depending on the shield. Such a difficult shielding calculation required advanced variance reduction. ADVANTG has some missing features, which limits its usability in spallation neutron source applications. It does not support volumetric sources created for MCNP6.2 UM capability. An approximate source was created for this problem. Not only was this approximate source needed for running the ADVANTG calculation to generate the weight windows, but also it was essential to develop source biasing (SB) parameters that were crucial for dramatically accelerating the decay photon transport in this problem. With this approximate source, the analysis was completed in a very reasonable computational time, and the design of the STS remote-handling equipment was finalized. This paper compares the efficiency of Monte Carlo simulations with different weight window and SB parameters calculated using different approximate ADVANTG calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

SCALE Shielding Calculations for Advanced Reactor Accident Scenarios

The study results presented in this paper demonstrate the capabilities of the SCALE computer code for non–light water reactor (non-LWR) radiation source term and shielding calculations in support of the U.S. Nuclear Regulatory Commission non-LWR fuel cycle demonstration project. Representative non-LWR types, including the sodium-cooled fast reactor (SFR), the molten salt reactor (MSR), and the heat pipe microreactor (HPMR), were analyzed to evaluate dose rates associated with postulated accident scenarios (SFR and MSR), reactor operation (MSR and HPMR), and fuel self-protecting characteristics (HPMR). New features were implemented in SCALE depletion codes to better simulate MSR operation.

MSR↗

DOE OSTI2021

A million persons, a million dreams: a vision for a national center of radiation epidemiology and biology

Epidemiologic studies of radiation-exposed populations form the basis for human safety standards. Furthermore, they also help shape public health policy and evidence-based health practices by identifying and quantifying health risks of exposure in defined populations. For more than a century, epidemiologists have studied the consequences of radiation exposures, yet the health effects of low levels delivered at a low-dose rate remain equivocal.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

DOE OSTI2023

Effects of ionising radiation exposure in offspring and next generations: dosimetric aspects and uncertainties

The impact of the exposure to ionizing radiation in the offspring and next generation has been investigated in the last decades and currently is the subject of study of the ICRP Task Group 121. Studying the effects of radiation exposure in pre-conceptional and post-conceptional phases can be a challenge since potential effects to the fetus vary depending on the stage of fetal development. Epidemiology and radiobiology studies are the two sources of information one can use to correlate the radiation dose to the human body and tissues and the resulting effects. For a proper evaluation of the outcomes of such studies, and a correct appraisal of the exposure/dose-effect relationship, (i) reliable dosimetry, (ii) accurate reporting, and (iii) reproducibility of results are required. Although variables related to dose, including for instance source of radiation, geometry of irradiation, dose rate etc., are usually known, especially in radiobiology studies, often important details of the irradiation are not reported. In conclusion, based on standards developed by the National Cancer Institute (NCI), the National Institute of Allergy and Infectious Disease (NIAID) and the National Institute of Standards and Technology (NIST), a review of the scientific studies used by the UNSCEAR to estimate the risk of hereditary effects, and by the ICRP in its current recommendations, was conducted to evaluate the way dosimetry was reported. Dosimetry and the related uncertainties were not adequately described in the vast majority of those studies. This does not necessarily mean that they do not provide relevant information, however it prevents from a thorough verification and reproduction of their findings. In order to guarantee the reliability and robustness of the process of revision of the estimates of risk and detriment it is therefore considered mandatory to include a careful check of the new relevant literature with regard to the criteria on the completeness and reproducibility of the dosimetric information.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

DOE OSTI2025

Towards Mitigating Electron Beam-Induced Damage in MOFs Using Low Dose Electron Microscopy for In-Situ Room-Temperature Measurements

Metal-Organic Frameworks (MOFs) have emerged as a versatile class of materials with applications in gas storage and separation, catalysis, and drug delivery [1]. Understanding their damage mechanisms in under various environmental conditions is crucial for optimizing performance and stability [2]. This study employs a combination of Length Structural Coherence (LSC) analysis in electron scattering and Electron Energy Loss Spectroscopy (EELS) to elucidate the damage mechanisms in two representative MOFs. MIL101(Fe), and MIL101(Cr). Here, the primary objective is to reveal structural and chemical changes that occur under electron beam irradiation in Scanning Transmission Electron Microscopy (STEM), both in the pristine state and during in-situ CO and CO 2 adsorption. By combining LSC in Radial Distribution Function (RDF) analysis with EELS, comprehensive insights into the nanoscale alterations are obtained and correlated to the electron dose rate.

dos Santos, Gabriel T. [Northwestern University, E↗

DOE OSTI2023

Deep Learning Approach for High-accuracy Electron Counting of Monolithic Active Pixel Sensor-type Direct Electron Detectors at Increased Electron Dose

Abstract Electron counting can be performed algorithmically for monolithic active pixel sensor direct electron detectors to eliminate readout noise and Landau noise arising from the variability in the amount of deposited energy for each electron. Errors in existing counting algorithms include mistakenly counting a multielectron strike as a single electron event, and inaccurately locating the incident position of the electron due to lateral spread of deposited energy and dark noise. Here, we report a supervised deep learning (DL) approach based on Faster region-based convolutional neural network (R-CNN) to recognize single electron events at varying electron doses and voltages. The DL approach shows high accuracy according to the near-ideal modulation transfer function (MTF) and detector quantum efficiency for sparse images. It predicts, on average, 0.47 pixel deviation from the incident positions for 200 kV electrons versus 0.59 pixel using the conventional counting method. The DL approach also shows better robustness against coincidence loss as the electron dose increases, maintaining the MTF at half Nyquist frequency above 0.83 as the electron density increases to 0.06 e−/pixel. Thus, the DL model extends the advantages of counting analysis to higher dose rates than conventional methods.

Materials Science↗

DOE OSTI2026

Distribution of Natural Radionuclides at the Nevada National Security Site

According to the United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) publications, contributions of terrestrial gamma doses are mainly from the presence of 40 K, and of 238 U and 232 Th together with their progeny in various rocks and soils. A survey of soil distributions of radionuclides 40 K, 238 U, and 232 Th was performed at the Nevada National Security Site (NNSS) using in situ gamma-ray spectrometry with a high-purity germanium (HPGe) detector. The average activity concentrations of 40 K, 238 U, and 232 Th in natural soils at the NNSS are 867 Bq kg -1 (range from 150 ± 8 to 1297 ± 56 Bq kg -1 ), 50 Bq kg -1 (range from 29 ± 3 to 74 ± 8 Bq kg -1 ), and 56 Bq kg -1 (range from 11 ± 2 to 96 ± 10 Bq kg -1 ), respectively. The concentration at each location is significantly associated with its geological lithology. The terrestrial gamma dose rates around the NNSS were estimated from 26 to 144 nSv h -1 with mean value of 93 nSv h -1 . In conclusion, our results provide useful information about the natural background radiation and radiological effects of naturally occurring radionuclides at the NNSS.

environmental assessment↗

DOE OSTI2021

FMX – the Frontier Microfocusing Macromolecular Crystallography Beamline at the National Synchrotron Light Source II

Two new macromolecular crystallography (MX) beamlines at the National Synchrotron Light Source II, FMX and AMX, opened for general user operation in February 2017 [Schneider et al. (2013). J. Phys. Conf. Ser. 425 , 012003; Fuchs et al. (2014). J. Phys. Conf. Ser. 493 , 012021; Fuchs et al. (2016). AIP Conf. Proc. SRI2015 , 1741 , 030006]. FMX, the micro-focusing Frontier MX beamline in sector 17-ID-2 at NSLS-II, covers a 5–30 keV photon energy range and delivers a flux of 4.0 × 10 12 photons s −1 at 1 Å into a 1 µm × 1.5 µm to 10 µm × 10 µm (V × H) variable focus, expected to reach 5 × 10 12 photons s −1 at final storage-ring current. This flux density surpasses most MX beamlines by nearly two orders of magnitude. The high brightness and microbeam capability of FMX are focused on solving difficult crystallographic challenges. The beamline's flexible design supports a wide range of structure determination methods – serial crystallography on micrometre-sized crystals, raster optimization of diffraction from inhomogeneous crystals, high-resolution data collection from large-unit-cell crystals, room-temperature data collection for crystals that are difficult to freeze and for studying conformational dynamics, and fully automated data collection for sample-screening and ligand-binding studies. FMX's high dose rate reduces data collection times for applications like serial crystallography to minutes rather than hours. With associated sample lifetimes as short as a few milliseconds, new rapid sample-delivery methods have been implemented, such as an ultra-high-speed high-precision piezo scanner goniometer [Gao et al. (2018). J. Synchrotron Rad. 25 , 1362–1370], new microcrystal-optimized micromesh well sample holders [Guo et al. (2018). IUCrJ , 5 , 238–246] and highly viscous media injectors [Weierstall et al. (2014). Nat. Commun. 5 , 3309]. The new beamline pushes the frontier of synchrotron crystallography and enables users to determine structures from difficult-to-crystallize targets like membrane proteins, using previously intractable crystals of a few micrometres in size, and to obtain quality structures from irregular larger crystals.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Sequential versus Simultaneous Aging of EPDM Nuclear Cable Insulation Subjected to Elevated Temperature and Gamma Radiation

Electrical cables are integral to power, control, and instrumentation systems within nuclear power plants (NPPs). Exposure of cable systems within nuclear containment to elevated temperatures and gamma radiation during decades-long operation of NPPs can lead to degradation of cable polymeric insulation. Prediction of nuclear cable insulation degradation is complicated as thermal and radiation stress are not additive. In this work, we explore the relative effects of simultaneous and sequential thermal and gamma irradiation on the aging of ethylene-propylene-diene (EPDM) elastomer insulation to better understand realistic scenarios of cable insulation degradation. Cable insulation samples of EPDM were subjected to up to 320 kGy of gamma radiation at a dose rate of 300 Gy/hr in two heating scenarios: (1) simultaneously aged samples were heated at 150°C during irradiation and (2) sequentially aged samples were heated at 150°C for designated durations followed by corresponding periods of irradiation at ambient temperature. The mass, tensile elongation at break, and carbonyl index were assessed to quantify aging of the polymers. The simultaneous aging scenario was found to the more severe of the two for EPDM insulation degradation.

ethylene-propylene-diene elastomer, EPDM, nuclear ↗

DOE OSTI2020

Sequential versus Simultaneous Aging of XLPE Nuclear Cable Insulation Subjected to Elevated Temperature and Gamma Radiation

Electrical cables constitute a critical component of nuclear power generation. The aging behavior of electrical cable insulation under combined exposure to thermal and radiation stress is not additive, complicating lifetime prediction of cable performance based on sequential accelerated aging. In this work we explore the relative effects of simultaneous and sequential thermal and gamma radiation aging on cross-linked polyethylene (XLPE), which is commonly found in commercial nuclear power plants in the United States. Samples of XLPE were subjected to up to 320 kGy of gamma irradiation at a dose rate of 300 Gy/hr in two heating scenarios. In the first, simultaneously-aged samples were heated at 150°C during irradiation. In the second, sequentially aged samples were heated at 150°C for designated durations followed by corresponding periods of irradiation without heating. The mass, total color difference, and density were characterized to quantify aging of the insulation polymer. Sequential aging is hypothesized to be more damaging to XLPE insulation due to an increased trend in mass gain, total color difference, and density.

Cross-linked polyethylene, XLPE, nuclear cable, ac↗

DOE OSTI2021

Principal Component Analysis of Nuclear Cable Insulation Subjected to Elevated Temperature and Gamma Radiation

In nuclear power plants (NPPs), the aging of electrical cable insulation occurs due to elevated temperature, ionizing radiation, and other environmental factors. To ensure the safe and efficient operation of NPPs, determination of key indicators of cable aging is critical to predict the remaining useful lifetime of electrical cable insulation. In this work, the effects of simultaneous and sequential thermal and gamma radiation on the aging of cross-linked polyethylene (XLPE) electrical cable insulation are investigated. The chemical changes of the insulation were monitored non-destructively through the use of Fourier transform infrared (FTIR) spectroscopy. The FTIR spectra were measured stepwise after predetermined exposure intervals, with a total irradiation dose up to 320 kGy at a dose rate of 300 Gy/hr in two exposure scenarios; simultaneously aged samples were heated at 150 °C during irradiation, while sequentially aged samples were heated at 150 °C for designated durations followed by corresponding times of irradiation at ambient temperature. A data-driven approach using principal component analysis (PCA) was developed to highlight changes in the carbonyl region of the infrared spectra of the aged samples due to oxidation and to differentiate oxidation rates under the simultaneous and sequential exposure conditions. Findings indicate that the sequential aging scenario may be more conservative than the simultaneous aging scenario for XLPE electrical cable insulation.

Li, Donghui↗