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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Visible to near-infrared spectral reflectance along the NGEE-Arctic tram transect, Utqiagvik (Barrow), Alaska, 2015-2018

Canopy spectral reflectance collected measured in 2015-2018 along the NGEE-Arctic tram located on the Barrow Environmental Observatory (BEO), Barrow, Alaska. Measurements were made using a PP-Systems UniSpec-DC spectrometer mounted on an automatically operated instrument cart. Spectra were collected at 137 stop points at 0.5 m intervals along the tram transect. Transect runs were collected daily, or multiple times per day, from April or May through to August or September each year. Downwelling radiance was measured using a 2 meter fiber optic cable connected to a cosine diffuser. Upwelling (i.e. reflected) radiance was measured using a 2 meter cable connected to a 12 degree field-of-view (FOV) lens. Canopy reflectance was calculated using the ratio of upwelling to downwelling radiance measured over a 99.99% reflectance Spectralon standard measured at the start of each measurement set. Unprocessed spectral data are presented in .spu files. Metadata are provided in csv files, and the instrument manual (pdf). The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was a 15-year research effort (2012-2027) to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy's Office of Biological and Environmental Research. The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska. Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Landscape-scale Characterization of Arctic Tundra Vegetation Composition, Structure, and Function with a Multi-sensor Unoccupied Aerial System: Supporting Data.

Airborne remote sensing data collected using the Brookhaven National Laboratory's (BNL) heavy-lift unoccupied aerial system (UAS) octocopter platform, the Osprey, operated by the Terrestrial Ecosystem Science and Technology (TEST) group (https://www.bnl.gov/testgroup). This package includes data from three flights flown over the NGEE-Arctic Council, Kougarok and Teller sites in July, 2018. The Osprey is a multi-sensor UAS platform that simultaneously measures very high spatial resolution optical red/green/blue (RGB) and thermal infrared (TIR) surface 'skin' temperature imagery, as well as surface reflectance at 1 nm intervals in the visible to near-infrared spectral range 350 - 1000 nm measured at regular intervals along each flight path. Derived image products include ortho-mosaiced RGB and TIR images, an RGB-based digital surface model (DSM) using the structure from motion (SfM) technique, digital terrain model (DTM), and a canopy height model (CHM). In addition, a VNIR surface reflectance file is provided for the trigger locations collected during each flight campaign. Ancillary aircraft data, flight mission parameters, and general flight conditions provided by the onboard flight and data collection computers are also included. Unprocessed and processed data products are included in this package (processing levels 0-3). Data and metadata are provided as text (*.txt, *.json, *.kml, *hdr, *.enp), tabular (*.dat, *.csv, *.waypoint, ENVI format (no extension)), point cloud (*.laz) and image (*.jpg, *.tif, *png) formats. This metadata document contains flight campaign, instrument and file metadata, along with a description of data processing levels, data products and file naming scheme.The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), a research effort to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy?s Office of Biological and Environmental Research.The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska.Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

UAS remote sensing (3DR SOLO platform): multispectral reflectance and normalized difference vegetation index, Seward Peninsula, Alaska, 2022

Airborne remote sensing data collected using a Parrot Sequoia+ multispectral sensor installed on a 3DR SOLO unoccupied aerial system (UAS) – operated by the Terrestrial Ecosystem Science & Technology group https://www.bnl.gov/envsci/testgroup/ at Brookhaven National Laboratory. This package includes data from 19 flights flown over the NGEE-Arctic, Kougarok Mile Marker (MM) 80, Kougarok Fire Complex (KFC) and Teller MM 27 sites in July 2022. Derived image products include point cloud, ortho-mosaiced multispectral image, a digital surface model (DSM) using the structure from motion (SfM) technique, and a normalized difference vegetation index (NDVI) map. Unprocessed and processed data products are included in this package (processing levels 0-2). Data and metadata are provided as text (*.txt, *.json, *hdr,), tabular (*.dat, *.csv), point cloud (*.laz), Cloud Optimized GeoTIFF (COG, *.tif), and image (*.jpg, *.tif, *png) formats.The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was a research effort to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy's Office of Biological and Environmental Research. The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska. Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

UAS remote sensing (3DR SOLO platform): multispectral reflectance, canopy height model, normalized difference vegetation index, Seward Peninsula, Alaska, 2021

Airborne remote sensing data collected using a Parrot Sequoia+ multispectral sensor installed on a 3DR SOLO unoccupied aerial system (UAS) - operated by the Terrestrial Ecosystem Science Technology group at Brookhaven National Laboratory. This package includes data from 10 flights flown over the NGEE-Arctic Council Mile Marker (MM) 71, Kougarok MM64, and Teller MM27 sites on the Seward Peninsula, Alaska, in August 2021. Derived image products include point cloud, ortho-mosaiced multispectral image, ortho-mosaiced RGB image, a digital surface model (DSM) using the structure from motion (SfM) technique, a canopy height model (CHM), and a normalized difference vegetation index (NDVI) map. Unprocessed and processed data products are included in this package (processing levels 0-2). Data and metadata are provided as text (*.txt, *.json, *hdr,), tabular (*.dat, *.csv), point cloud (*.laz), Cloud Optimized GeoTIFF (COG, *.tif), and image (*.jpg, *.tif, *png) formats. The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was a research effort to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy's Office of Biological and Environmental Research. The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska. Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Canopy spectral reflectance, Kougarok and Teller sites, Seward Peninsula, Alaska, 2016

Measurements of full-spectrum (350-2500 nm) canopy spectral reflectance of Arctic plant species at the Teller and Kougarok NGEE-Arctic sites, Seward Peninsula, Alaska. Spectra were collected in July 2016 using an SVC HR-2014i spectroradiometer together with a Spectralon white plate to calibrate each measurement under variable illumination conditions. The locations of the 43 measurement targets are provided as latitude and longitude recorded by the spectroradiometer internal GPS. This data package comprises .csv data and metadata files, and the SVC instrument output (.sig in .zip). The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was a research effort to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy's Office of Biological and Environmental Research. The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska. Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy's Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

n-Propylbenzene Droplet Combustion: Experiments and Numerical Modeling

n-Propylbenzene (PB, C9H12, 432K boiling point) is important as a constituent in surrogates for some transportation fuels but little is understood about its droplet burning characteristics. We present an experimental and numerical study of a fuel droplet burning under conditions where the sole means of gas transport is fuel evaporation at the droplet surface thereby creating a one-dimensional gas transport that is amenable to detailed numerical modeling. The one-dimensional gas transport that results is amenable to detailed numerical modeling. Initial droplet diameters (Do) ranged from 0.3 mm to about 5 mm to better understand the mechanisms that control burning over such a wide range of Do. For Do < 1 mm droplets were burned while anchored to 14 m SiC fibers within a sealed container in free-fall during which time the droplets were ignited by spark discharge and the burning process recorded by video cameras. Larger and free-floating droplets were studied in the spaced-based platform of the orbiting International Space Station for Do > 1.0 mm which provided unlimited times for experimental observation. Measurements of droplet, flame and soot shell diameters were made and are discussed in the presentation. The experimental results showed formation of optically thick soot clouds developing during burning that required a robust image analysis algorithm to enable measurement of droplet diameter. The measured droplet diameters were well predicted by a numerical model that included soot formation, a PB kinetic mechanism comprising 576 species and 27369 reactions, unsteady gas and liquid transport, variable properties and radiative transport. Flame diameters showed more variability compared to the simulations, depending on how the flame was defined (peak gas temperature and OH concentration). Droplets burned slower as Do was increased and the PB sooting propensity increased with Do. Flame extinction was observed for Do > 3.3 mm indicating a strong effect of radiation as Do was increased compared to the smaller droplet diameters examined where extinction was not experimentally observed. For the largest droplets examined the possibility that the observed extinction is indicative of a transition to cool flame burning is still under investigation.

Guo, Songtao↗
DOE OSTI2024

Towards higher frequencies in a compact prebunched waveguide THz-FEL

Free-electron-lasers fill a critical gap in the space of THz-sources as they can reach high average and peak powers with spectral tunability. Using a waveguide in a THz FEL significantly increases the coupling between the relativistic electrons and electromagnetic field enabling large amounts of radiation to be generated in a single passage of electrons through the undulator. In addition to transversely confining the radiation, the dispersive properties of the waveguide critically affect the velocity and slippage of the radiation pulse which determine the central frequency and bandwidth of the generated radiation. In this paper, we characterize the spectral properties of a compact waveguide THz FEL including simultaneous lasing at two different frequencies and demonstrating tuning of the radiation wavelength in the high frequency branch by varying the beam energy and ensuring that the electrons injected into the undulator are prebunched on the scale of the resonant radiation wavelength.

Experimental particle physics↗
DOE OSTI2020

Novel complex ceramic oxides, Ln 2 TiO 5 (Ln = La, Sm, Gd, Tb, Dy, Ho, Er, and Yb), for polyphase nuclear waste‐forms

Abstract As part of a broader study of ceramic nuclear waste‐forms, four different lanthanide titanates were fabricated; La 0.1 Sm 0.1 Gd 0.1 Tb 0.1 Dy 0.3 Ho 0.1 Er 0.2 YbTiO 5 , Sm 0.3 Gd 0.3 Dy 0.3 Yb 1.1 TiO 5 , Sm 0.1 Gd 0.4 Dy 0.4 Yb 1.1 TiO 5 , and Sm 0.2 Gd 0.2 Dy 0.2 Yb 1.4 TiO 5 . The aim was to produce single‐phase novel materials with cubic symmetry, capable of incorporating a wide variety of cations and with acceptable radiation tolerance. The chemistry flexibility and radiation tolerance are some of the major desirable properties for nuclear waste‐form materials. By using multiple lanthanides the average lanthanide radius can be controlled and consequently the structure, along with properties such as radiation tolerance. The radiation tolerance was assessed using in situ 1 MeV krypton irradiation and transmission electron microscopy characterization. Those materials for which cubic symmetry was achieved displayed better radiation tolerance; a greater critical fluence of ions ( F c ) was required for the crystalline to amorphous transition, and a lower temperature was required to maintain crystallinity ( T c ) during irradiation.

Aughterson, Robert D.↗
DOE OSTI2021

Evaluation and improvement of the parameterization of aerosol hygroscopicity in global climate models using in-situ surface measurements (Final Report)

Aerosols are tiny particles suspended on the atmosphere that can interact with incoming solar radiation and affect the Earth radiative budget. They do so by scattering and absorbing solar radiation, and these properties vary depending on the aerosol size and chemical composition. Moreover, by taking up water from the surrounding air, hygroscopic aerosol particles will grow in size and change their chemical composition, thus modifying their optical properties (scattering and absorption) and their final impact on radiative forcing calculations. An accurate knowledge of aerosol hygroscopicity is crucial for estimating the net radiative impact of aerosols. We took a three-pronged approach to improve our understanding of aerosol hygroscopicity and how it is implemented in Earth system models. In the first part of our project, we developed a benchmark dataset from existing aerosol hygroscopic growth measurements made by tandem nephelometer humidogram systems. We analyzed, using a standardized methodology, observations from 26 in-situ stations around the globe. Measurement data was collected from multiple data providers, reviewed and harmonized to create a consistent dataset of the scattering enhancement factor due to aerosol water uptake. This dataset is archived in several publicly available databases for use by interested researchers. In the second part of the project, we used the benchmark hygroscopicity dataset to perform a global study on aerosol hygroscopicity and aerosol optical properties. Measurements show a global picture of scattering enhancement with larger values for Arctic and marine sites and lower for urban and desert sites. We assessed the RH dependence of aerosol radiative forcing and showed that the overall effect of aerosol hygroscopicity on DARF is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 compared to dry conditions (RH<40%). Finally, we explored using aerosol single scattering albedo (SSA) and scattering Angstrom exponent (SAE) as possible proxies for aerosol hygroscopicity. SSA showed more promise as a surrogate for the scattering enhancement factor than SAE, but neither was ideal. In the third part of the project we evaluated the output of ten Earth system models (ESMs) against the benchmark hygroscopicity dataset. ESMs utilize various schemes for aerosol hygroscopicity which had not been previously tested against observations on a global scale. We found that ESMs currently overestimate scattering enhancement due to hygroscopic growth. Model parameterizations of hygroscopicity and model chemistry are two main factors driving the observed diversity in hygroscopicity simulations among the models. In addition, our study makes several suggestions for modelers, including improving the parameterizations of organic and sea salt aerosol hygroscopicity. Future hygroscopicity model evaluation experiments should include the model data related to particles size which was not available for our study.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Connecting radiation-driven changes in structural, thermal, and mechanical properties in several medical device polymers

Stemming from security threats and shortages in supply, a recent push has emerged to develop alternatives to radioisotope Cobalt-60 gamma radiation for sterilization of polymeric medical products, including electron beam (e-beam) and X-ray machine-based sources. However, before large-scale implementation, the effects of these non-isotope-based methods must be thoroughly investigated from several perspectives, involving their potential detrimental effects on the structural, thermal, and mechanical properties of polymers in medical devices. This paper investigates such effects in commonly used medical device polymers, including polypropylene homopolymer (PPH), polyolefin elastomer (POE), low-density polyethylene (LDPE), acrylonitrile butadiene styrene (ABS), and chlorobutyl rubber (CIIR). To connect radiation-driven changes in polymer structural and thermal properties and corresponding changes in mechanical properties, several characterization techniques were utilized, including gel permeation chromatography (GPC), Fourier transform infrared spectroscopy (FTIR), dynamic mechanical analysis (DMA) and differential scanning calorimetry (DSC). We found that the tensile strength of X-ray irradiated PPH, as well as X-ray, e-beam, and gamma irradiated CIIR decreases due to chain scission, which is corroborated by GPC and DMA. The GPC results of LDPE suggest chain scission, but interestingly without a corresponding decline in tensile strength. By comparison, POE and ABS appear to undergo further crosslinking with increasing irradiation dose, which generally strengthens them. Importantly, in the vast majority of the cases, there were small to no changes in properties upon changing radiation technologies (at a given dose), i.e., no radiation source dependence. However, in a few specific cases, radiation method dependencies did arise, for instance, in terms of the molecular weight of PPH being significantly increased upon X-ray irradiation, while the melting temperature, glass transition temperature, and elongation at break reduced compared to gamma. Overall, this study provides valuable insight into radiation-driven chemical and structural changes in polymers that produce changes in physical and functional properties.

36 MATERIALS SCIENCE↗
DOE OSTI2021

The Shortwave Spectral Radiometer for Atmospheric Science: Capabilities and Applications from the ARM User Facility

Industry advances have greatly reduced the cost and size of ground-based shortwave (SW) sensors for the ultraviolet, visible, and near-infrared spectral ranges that make up the solar spectrum, while simultaneously increasing their ruggedness, reliability, and calibration accuracy needed for outdoor operation. These sensors and collocated meteorological equipment are an important part of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility, which has supported parallel integrated measurements of atmospheric and surface properties for more than two decades at fixed and mobile sites around the world. The versatile capability of these ground-based measurements includes 1) rich spectral information required for retrieving cloud and aerosol microphysical properties, such as cloud phase, cloud particle size, and aerosol size distributions, and 2) high temporal resolution needed for capturing fast evolution of cloud microphysical properties in response to rapid changes in meteorological conditions. Here we describe examples of how ARM's spectral radiation measurements are being used to improve understanding of the complex processes governing microphysical, optical, and radiative properties of clouds and aerosol.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Investigations of radiation damaged arranged scintillating particle composites

Composites consisting of periodically arranged scintillating particles within an acrylic (poly methyl methacrylate) matrix are excellent templates for the gamma-insensitive detection of fast neutrons. In order to study the impact of radiation damage on acrylic-based scintillating particle composites, we exposed acrylic samples to different doses of fast neutrons up to 119.7 kGy and investigated the change in optical characteristics using optical absorption spectroscopy in the 200–800 nm wavelength range. The experimental results are compared to coupled MCNP6 and optical ray-tracing (FRED) simulations, and qualitative agreement is found. Neutron-induced radiation damage in the acrylic matrix manifests as a red-shift in the ultra-violet absorption edge of the acrylic and a corresponding decrease in the light propagation efficiency, which leads to detector performance degradation. We show for the first time that the effects of radiation damage can be mitigated by the use of wavelength-shifting coatings. We predict that composites with wavelength-shifting coatings can enable neutron detectors with high tolerance against neutron-induced radiation damage, a property that is particularly desired for neutron detection in high radiation environments.

36 MATERIALS SCIENCE↗
DOE OSTI2023

The effects of radiation-induced grain subdivision and dislocations on the fracture properties of uranium dioxide

Microcantilever bending tests were applied on uranium dioxide samples irradiated by 84 MeV Xe ions. Depending on the initial grain sizes, different levels of grain subdivision and dislocation development were observed near the irradiated surface. These radiation damage features were shown to degrade the fracture properties of both samples. The fundamental aspects of the radiation-microstructure-property relationships were discussed in this paper, taking a holistic consideration of the microcantilever bending data, fractography and microstructures. The separate effects of the irradiation-induced grain subdivision and dislocations on the fracture initiation and propagation of uranium dioxide were discussed. In conclusion, it was observed that radiation-induced dislocations and grain subdivision, without the presence of Xe bubbles co-located with the defects, cause reductions in the Young's modulus, fracture strain, and fracture stress, and a transition to intergranular fracture.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Unveiling and Mapping Polymorphs in Fluorite Y2TiO5 Using 4D-STEM and Unsupervised Machine Learning

Y2TiO5 belongs to the Ln2TiO5 (Ln = lanthanide or Y) family of ceramic materials and exhibits a range of desirable material properties such as radiation tolerance, frustrated magnetism, and large dielectric constant. However, understanding the complex crystal structure of Y2TiO5 remains elusive, given that Y2TiO5 can adopt multiple polymorphs such as cubic, orthorhombic, and hexagonal phases within the lattice. In this work, we report a detailed structural analysis of Y2TiO5 using four-dimensional scanning transmission electron microscopy coupled with unsupervised machine learning. The pyrochlore nanodomains, characterized by the ordered arrangement of yttrium cations on the A site of their A2BO5 structure, are present within the matrix of a predominantly fluorite-structured Y2TiO5 along with a third polymorph, the hexagonal phase. The pyrochlore phase is found to form 2 nm boundary regions around hexagonal phase stacking faults, highlighting the potential influence of the hexagonal phase on the occurrence and distribution of the pyrochlore phase. Lastly, we identify a unique pyrochlore phase with asymmetric arrangement of cation ordering along a single planar direction. Our findings provide invaluable insights into the possible mechanisms stabilizing pyrochlore nanodomains within the fluorite lattice of Y2TiO5.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Radiation-Induced Effects on the Extraction Properties of Hexa-n-octylnitrilo-triacetamide (HONTA) Complexes of Americium and Europium

The candidate An(III)/Ln(III) separation ligand hexa-n-octylnitrilo-triacetamide (HONTA) was irradiated under envisioned SELECT (Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation) process conditions (n-dodecane/0.1 M HNO 3 ) using a solvent test loop in conjunction with cobalt-60 gamma irradiation. The extent of HONTA radiolysis and complimentary degradation product formation was quantified by HPLC-ESI-MS/MS. Further, the impact of HONTA radiolysis on process performance was evaluated by measuring the change in 243 Am and 154 Eu distribution ratios as a function of absorbed gamma dose. HONTA was found to decay exponentially with increasing dose, affording a dose coefficient of d = (4.48 ± 0.19) × 10 –3 kGy –1 . Multiple degradation products were detected by HPLC-ESI-MS/MS with dioctylamine being the dominant quantifiable species. Both 243 Am and 154 Eu distribution ratios exhibited an induction period of ~70 kGy for extraction (0.1 M HNO 3 ) and back-extraction (4.0 M HNO 3 ) conditions, after which both values decreased with absorbed dose. The decrease in distribution ratios was attributed to a combination of the destruction of HONTA and ingrowth of dioctylamine, which is capable of interfering in metal ion complexation. Furthermore, the loss of HONTA with absorbed gamma dose was predominantly attributed to its reaction with the n-dodecane radical cation (R˙ + ). These R˙ + reaction kinetics were measured for HONTA and its 241 Am and 154 Eu complexes using picosecond pulsed electron radiolysis techniques. All three second-order rate coefficients (k) were essentially diffusion limited in n-dodecane indicating a significant reaction pathway: k(HONTA + R˙ + ) = (7.6 ± 0.8) × 10 9 M –1 s –1 , k(Am(HONTA) 2 + R˙ + ) = (7.1 ± 0.7) × 10 10 M –1 s –1 , and k(Eu(HONTA) 2 + R˙ + ) = (9.5 ± 0.5) × 10 10 M –1 s –1 . HONTA-metal ion complexation afforded an order-of-magnitude increase in rate coefficient. Additional nanosecond time-resolved measurements showed that both direct and indirect HONTA radiolysis yielded the short-lived (< 100 ns) HONTA radical cation and a second long-lived (µs) species identified as the HONTA triplet excited state. The latter was confirmed by a series of oxygen quenching picosecond pulsed electron measurements, affording a quenching rate coefficient of k( 3 [HONTA]* + O 2 ) = 2.2 × 10 8 M –1 s –1 . Overall, both the HONTA radical cation and triplet excited state are important precursors to the suite of measured HONTA degradation products.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Radiation damages the silicates present in polyphasic mineral aggregates causing concrete’s degradation

While many U.S. nuclear power plants have submitted Subsequent License Renewal Application to operate beyond 60 years, others are already considering Operations Beyond Eighty years. In such cases, concrete biological shields are exposed to neutron and gamma radiation exceeding prescribed thresholds. Radiation-induced volumetric expansion (RIVE), extensively studied in single crystals, may also contribute to the degradation of polycrystalline aggregates. Since minerals differ in atomic structure and chemistry, radiation can affect them in distinct ways. This study examines quartzite, marble, and limestone to evaluate how irradiation affects their physical attributes and chemical reactivity. Results show crystalline silicates experience significant RIVE damage and enhanced reactivity in alkaline solutions compared to non-irradiated phases. Enhanced intra- and inter-granular dissolution could compromise aggregate integrity. An empirical correlation links silicate dissolution rate to atomic constraints (density, rigidity) and radiation dose, providing a predictive framework for estimating changes in silicate aggregate properties within radiation-exposed concrete.

Bouissonnié, Arnaud [Univ. of California, Los Ange↗