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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Structural Properties of Ditechnetium Heptoxide, Tc{sub 2}O{sub 7}

Group 7 elements form unique binary oxides with the stoichiometry M{sub 2}O{sub 7}. The heptoxides of manganese and technetium crystallize as molecular solids while rhenium forms an extended solid with mixed valances, 4 and 6. Unlike manganese and rhenium heptoxides which are used in the chemical industry technetium heptoxide has found very few applications due to its radioactive nature; it has been primarily use as a chemical precursor. While both of the molecular solids, Mn{sub 2}O{sub 7}{sup 3} and Tc{sub 2}O{sub 7}{sup 4} can be described by two corner-sharing MO{sub 4} tetrahedron. The most distinctive difference is that the manganese's compound has a metal-oxygen-metal bond angle of 120.7 deg. while the technetium species is 180 deg.. Additionally, Tc{sub 2}O{sub 7} has the largest molar volume of the heptoxides which suggest that it will be more susceptible to external stimuli of pressure and temperature than the others heptoxides. A pressure induced twisting has been predicted by Fang et al. Anomalous behavior is seen in the c-axis where below 2 GPa the Van der Waals interactions between the Tc{sub 2}O{sub 7} molecules is over come and compression is observed but at higher pressures the twisted distortion forces the lattice to expand. The terminology diagonal-double tetrahedrons (DDTs) is introduced to discuss the molecules of Tc{sub 2}O{sub 7}. The rigid nature of the DDTs has been attributed to the cause of this twisted distortion mechanism. Recently, the solid state and gas phase behavior of technetium heptoxide was revisited by Childs et al. in light of {sup 99}Tc being an important dose contributor in the Hanford waste and vitrification being proposed for immobilization of nuclear waste. Technetium heptoxide is one of the proposed volatilized species of technetium found in the vitrification process. In this study the crystal structure of Tc{sub 2}O{sub 7} was reported at 100 K and compared to the structure first determined by Krebs at room temperature. Inspection of the metal-oxygen distances revealed the 100 K structure had longer bond lengths for the bridging oxygen than at high temperature. It is suggested that transverse thermal vibrational modes can be used to explain this negative thermal expansion behavior. This describes the average bond length of a central atom (i.e. the bridging oxygen atom) being measured as shorter at higher temperatures due to the larger thermal motion. Diffraction methods that measure the long range average structure are susceptible to observing this shorter average length as opposed to the true bond length, atom position at oscillation node that a method like Pair-Distribution Functional PDF Analysis would yield. In the case of Tc{sub 2}O{sub 7}, the magnitude of the transverse thermal vibrational mode is at the limit of being detectable by SCXRD and likely not observable by PDF analysis. Here we report the preliminary results of our study on the nature of the thermal expansion behavior of Tc{sub 2}O{sub 7}. The transverse thermal vibration mode compression mechanism is considered and compared to the pressure induced twisted distortion mechanism predicted at high pressure. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Investigating radioactive negative ion production via double electron capture

The relative cross sections for radioactive negative ion production via double electron capture have been measured for collisions between a 40 keV projectile beam of uranium-238 and potassium vapor. This was performed at the collinear resonance ionization spectroscopy (CRIS) experiment at CERN-ISOLDE and is a step towards measuring the electron affinities (EAs) of elements that cannot be efficiently produced in negative ion sources at radioactive ion beam (RIB) facilities. This includes short-lived radioactive isotopes that have low production quantities and heavy and superheavy elements that systematically have smaller EAs than work functions of available ion source materials. Negative ions are particularly sensitive to electron–electron correlation effects, which make such studies ideal for benchmarking atomic structure models that go beyond the independent particle model. While the EAs of most light elements have been measured, experimental investigations on heavier elements, namely the actinides, remain scarce due to their radioactive nature and production difficulty. By developing negative ion production by charge exchange, we aim to make these studies feasible at RIB facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Understanding Materials Characteristics of Palladium Lanthanide Cermet Wires as a Mimic of Californium Wire Production

Californium-252 (Cf-252) has been synthesized on a large scale (mg) since the 1970s for use as a portable neutron source. With a half-life of 2.645 years and a spontaneous fission fraction of 3.09%, Cf-252 emits 2.31 × 10 12 neutrons/gram second. Today most of the Cf-252 produced in the world is made at Oak Ridge National Laboratory (ORNL) using the High Flux Isotope Reactor (HFIR) and the Radiochemical Engineering Development Center (REDC). Because of its highly radioactive nature, all manipulations of Cf-252 need to be performed in hot cell facilities by highly trained personnel. The Cf-252 produced at ORNL is done at the REDC, which is conveniently located next to the HFIR. Cf-252 is sold as bulk wire, which has been described as palladium (Pd) metal incasing californium oxide (Cf 2 O 3 ). The process was developed by Mosley et al. at Savannah River Laboratory (SRL) where it was modeled after the thorium work done by Fuschillo et al. This process has been used since the 1970s to synthesize this unique wire, but its fundamental chemistry and materials characteristics were never openly reported. Here we aim to better understand the chemistry and the materials characteristics of Cf-252 wire production for process improvements and to better our fundamental understanding of the mid-late actinides. Though there are many challenges in working with radioactive elements such as Cf, the isotope Cf-252 is even more complicated due to its neutron emission. One challenge with neutron emission is the ability of neutrons to penetrate much deeper through materials, causing radiation damage. This makes using instrumentation to characterize the chemistry and materials properties of this process difficult. For this reason, this study will first focus on terbium (Tb) as a surrogate for Cf. Currently Tb is used as a carrier or filler in Cf production when small amounts of Cf are being processed. This, along with their similar size and charge, makes Tb a reasonable surrogate for this study.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Concept of an upright wearable positron emission tomography imager in humans

Abstract Background Positron Emission Tomography ( PET ) is traditionally used to image patients in restrictive positions, with few devices allowing for upright, brain‐dedicated imaging. Our team has explored the concept of wearable PET imagers which could provide functional brain imaging of freely moving subjects. To test feasibility and determine future considerations for development, we built a rudimentary proof‐of‐concept prototype (Helmet_ PET ) and conducted tests in phantoms and four human volunteers. Methods Twelve Silicon Photomultiplier‐based detectors were assembled in a ring with exterior weight support and an interior mechanism that could be adjustably fitted to the head. We conducted brain phantom tests as well as scanned four patients scheduled for diagnostic F 18‐ FDG PET / CT imaging. For human subjects the imager was angled such that field of view included basal ganglia and visual cortex to test for typical resting‐state pattern. Imaging in two subjects was performed ~4 hr after PET / CT imaging to simulate lower injected F 18‐ FDG dose by taking advantage of the natural radioactive decay of the tracer (F 18 half‐life of 110 min), with an estimated imaging dosage of 25% of the standard. Results We found that imaging with a simple lightweight ring of detectors was feasible using a fraction of the standard radioligand dose. Activity levels in the human participants were quantitatively similar to standard PET in a set of anatomical ROI s. Typical resting‐state brain pattern activation was demonstrated even in a 1 min scan of active head rotation. Conclusion To our knowledge, this is the first demonstration of imaging a human subject with a novel wearable PET imager that moves with robust head movements. We discuss potential research and clinical applications that will drive the design of a fully functional device. Designs will need to consider trade‐offs between a low weight device with high mobility and a heavier device with greater sensitivity and larger field of view.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2019

Radiogenic backgrounds in the NEXT double beta decay experiment

Natural radioactivity represents one of the main backgrounds in the search for neutrinoless double beta decay. Within the NEXT physics program, the radioactivity-induced backgrounds are measured with the NEXT-White detector. Data from 37.9 days of low-background operations at the Laboratorio Subterr\'aneo de Canfranc with xenon depleted in $^{136}$Xe are analyzed to derive a total background rate of (0.84$\pm$0.02) mHz above 1000 keV. The comparison of data samples with and without the use of the radon abatement system demonstrates that the contribution of airborne-Rn is negligible. A radiogenic background model is built upon the extensive radiopurity screening campaign conducted by the NEXT Collaboration. A spectral fit to this model yields the specific contributions of $^{60}$Co, $^{40}$K, $^{214}$Bi and $^{208}$Tl to the total background rate, as well as their location in the detector volumes. The results are used to evaluate the impact of the radiogenic backgrounds in the double beta decay analyses, after the application of topological cuts that reduce the total rate to (0.25$\pm$0.01) mHz. Based on the best-fit background model, the NEXT-White median sensitivity to the two-neutrino double beta decay is found to be 3.5$\sigma$ after 1 year of data taking. The background measurement in a Q$_{\beta\beta}\pm$100 keV energy window validates the best-fit background model also for the neutrinoless double beta decay search with NEXT-100. Only one event is found, while the model expectation is (0.75$\pm$0.12) events.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Selenium interaction with iron minerals: Quantitative comparison of sorption and coprecipitation impacts on mobility

Given the significance of selenium (Se) as a micronutrient, the radioactive nature of some of its isotopes, and its affinity to iron (Fe) minerals, extensive research has been conducted on the sorption mechanisms between Se and these minerals. Here, in this study, we employ sorption data sourced from the L-SCIE database and coprecipitation data from available literature to achieve the following objectives: i) establish coherence between adsorption and coprecipitation processes, ii) quantitatively evaluate the importance of these processes in nuclear waste repository science, and iii) propose a forward-looking approach for integrating coprecipitation into reactive transport models. Our findings indicate that a correlation between Se adsorption and coprecipitation can be established using the λ formalism. The comparable log(λ Se(IV) /λ Se(VI) ) ratios derived from adsorption and coprecipitation experiments suggest that these processes can be quantitatively compared and evaluated using our numerical approach. Across all iron oxide phases examined, coprecipitation leads to significantly greater immobilization of Se compared to adsorption. Specifically, for hydrous ferric oxide, hematite, and goethite, coprecipitation is predicted to result in 100–1000 times more Se immobilization compared to adsorption, irrespective of the Se oxidation state (Se(IV) or Se(VI)); notably stronger immobilization potential via coprecipitation was observed for magnetite. The modeling approach and quantitative analysis presented herein clearly highlight the importance of including coprecipitation processes when simulating Se (and other elements) transport, particularly under conditions where mineral compositions are transient or evolving with time. Neglecting coprecipitation in models is likely to lead to significant overestimates of migration.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Ab-Initio molecular dynamics simulations of binary NaCl-ThCl 4 and ternary NaCl-ThCl 4 -UCl 3 molten salts

Molten salt reactor (MSR) with Thorium (Th) fuel cycle has attracted growing attention due to its merits such as safety, low radioactive waste production, and non-proliferation. The design and safe operation of MSR rely on a thorough understanding of the thermophysical properties of molten salts over a wide range of composition and temperature. However, experimental data of Th-based molten salts are limited due to the inherent challenges of dealing with corrosive molten salts and the radioactive nature of actinides. Here, in this work, thermophysical properties including density, heat capacity, thermal expansion coefficient, and mixing energy of binary NaCl-ThCl 4 and ternary NaCl-ThCl 4 -UCl 3 molten salts are explored using ab-initio molecular dynamic simulations (AIMD) with the dDsC dispersion correction. The calculated mixing energy of binary NaCl-ThCl 4 exhibits a minimum close to the eutectic composition. The heat capacity of the mixtures is linearly dependent on the mole fraction of each component. 7-fold and 6-fold coordinated Th complexes are dominant in the mixtures. 8-fold coordinated Th complex increases with ThCl 4 fraction due to the formation of network structures. The average coordination number of Th exhibits a minimum near the eutectic composition. The minimum mixing energy for the ternary mixtures is observed in systems with a composition close to [NaCl] 0.5 [ThCl 4 ] 0.25 [UCl 3 ] 0.25 . The density positively deviates from the ideal solution in mixtures near this composition. These results are important to fill the data and knowledge gap of ThCl 4 molten salts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Quantification of Raman-Interfering Polyoxoanions for Process Analysis: Comparison of Different Chemometric Models and a Demonstration on Real Hanford Waste

The Hanford site represents a complicated environmental remediation challenge, remaining from the production of nuclear weapons. Over 100 million gallons of liquid radioactive waste of unknown composition will be chemically processed and vitrified, but the varying chemical composition and highly radioactive nature of the waste preclude the implementation of more developed, offline technologies to determine the composition. The only practical approach to waste treatment will require the significant utilization of real-time, chemometric modeling approaches. Although chemometric approaches have been applied to the analysis of Hanford waste, the models developed were highly tank-specialized, and limited discussion was provided on how models fared with interfering signals. As the tank waste is largely composed of oxoanions, which tend to have interfering Raman spectra, the general question was posed as to what chemometric approach is best suited to accurately quantify analytes in the presence of interfering signals. This was carried out by examining the ability of classical least square (CLS), principal component regression (PCR), partial least square (PLS), and locally weighted regression (LWR) to quantify NO 3 – and CO 3 2– using their bands around 1050 cm –1 . Finally, for all samples, the PLS-based model was found to be the most efficient approach from a model building and application perspective.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Technetium: The First Radioelement on the Periodic Table

The radioactive nature of technetium is discussed using a combination of introductory nuclear physics concepts and empirical trends observed in the chart of the nuclides and the periodic table of the elements. Trends such as the enhanced stability of nucleon pairs, magic numbers, and Mattauch's rule are described. Here, the concepts of nuclear binding energies and the nuclear shell model are introduced and used to explain the relative stability of radionuclides and, in particular, the isotopes of technetium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Simulation of charge readout with segmented tiles in nEXO

nEXO is a proposed experiment to search for the neutrino-less double beta decay (0νββ) of 136 Xe in a tonne-scale liquid xenon time projection chamber (TPC). The nEXO TPC will be equipped with charge collection tiles to form the anode. In this work, the charge reconstruction performance of this anode design is studied with a dedicated simulation package. A multi-variate method and a deep neural network are developed to distinguish simulated 0νββ signals from backgrounds arising from trace levels of natural radioactivity in the detector materials. These simulations indicate that the nEXO TPC with charge-collection tiles shows promising capability to discriminate the 0νββ signal from backgrounds. Furthermore, the estimated half-life sensitivity for 0νββ decay is improved by 20 32)% with the multi-variate (deep neural network) methods considered here, e sensitivity estimated in the nEXO pre-conceptual design report.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Contributions of Various Radiological Sources to Background in a Suburban Environment

This work is a brief overview and comparison of dose rates stemming from both indoor and outdoor natural background radiation and household objects within a suburban environment in North Carolina. Combined gamma and beta dose rates were taken from indoor objects that ranged from the potassium in fruit to the americium in smoke detectors. For outdoor measurements, various height and time data samples were collected to show fluctuations in dose rate due to temperature inversion and geometric attenuation. Although each sample tested proved to have a statistically significant increase over background using Students t-test, no sample proved to be more than a minor increase in natural radiation dose. Furthermore, the relative contributions from natural radioactivity such as potassium in foods and common household items are shown to be easily distinguished from background using standard handheld instrumentation when applied in a systematic, methodological manner.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2020

Results on low-mass weakly interacting massive particles from an 11 kg d target exposure of DAMIC at SNOLAB

We present constraints on the existence of weakly interacting massive particles (WIMPs) from a 11 kg-day target exposure of the DAMIC experiment at the SNOLAB underground laboratory. The observed energy spectrum and spatial distribution of ionization events with electron-equivalent energies $>$200 eV$_{\rm ee}$ in the DAMIC CCDs are consistent with backgrounds from natural radioactivity. An excess of ionization events is observed above the analysis threshold of 50 eV$_{\rm ee}$. While the origin of this low-energy excess requires further investigation, our data exclude spin-independent WIMP-nucleon scattering cross sections $\sigma_{\chi-n}$ as low as $3\times 10^{-41}$ cm$^2$ for WIMPs with masses $m_{\chi}$ from 7 to 10 GeV$c^{-2}$ . These results are the strongest constraints from a silicon target on the existence of WIMPs with $m_{\chi}$$<$9 GeV$c^{-2}$ and are directly relevant to any dark matter interpretation of the excess of nuclear-recoil events observed by the CDMS silicon experiment in 2013.

WIMP search, Dark Matter, DAMIC, SNOLAB↗
DOE OSTI2024

Measurement of the background in the CMS muon detector in ${p}{p}$-collisions at $\sqrt{s} = 13$ TeV

The CMS detector, including its muon system, has been operating at the CERN LHC in increasingly challenging conditions for about 15 years. The muon detector was designed to provide excellent triggering and track reconstruction for muons produced in proton–proton collisons at an instantaneous luminosity ($\mathcal{L}$) of 1 x 10 34 cm –2 s –1 . During the Run 2 data-taking period (2015–2018), the LHC achieved an instantaneous luminosity of twice its design value, resulting in larger background rates and making the efficient detection of muons more difficult. While some backgrounds result from natural radioactivity, cosmic rays, and interactions of the circulating protons with residual gas in the beam pipe, the dominant source of background hits in the muon system arises from proton–proton interactions themselves. Charged hadrons leaving the calorimeters produce energy deposits in the muon chambers. In addition, high-energy particles interacting in the hadron calorimeter and forward shielding elements generate thermal neutrons, which leak out of the calorimeter and shielding structures, filling the CMS cavern. We describe the method used to measure the background rates in the various muon subsystems. These rates, in conjunction with simulations, can be used to estimate the expected backgrounds in the High-Luminosity LHC. This machine will run for at least 10 years starting in 2029 reaching an instantaneous luminosity of $\mathcal{L}$ = 5 x 10 34 cm –2 s –1 and increasing ultimately to $\mathcal{L}$ = 7.5 x 10 34 cm –2 s –1 . These background estimates have been a key ingredient for the planning and design of the muon detector upgrade.

Tytgat, M. (ORCID:0000000239902074)↗
DOE OSTI2024

Development of selenium imaging detectors toward a definitive search for neutrinoless ββ decay

Imaging sensors made from an ionization target layer of amorphous selenium (aSe) coupled to a silicon complementary metal-oxide-semiconductor (CMOS) active pixel array for charge readout are a promising technology for neutrino physics. The high spatial resolution in a solid-state target provides unparalleled rejection of backgrounds from natural radioactivity in the search for the neutrinoless ββ decay of 82 Se. With this grant, we experimentally determined two crucial factors necessary for the realization of this novel technology: i) the intrinsic energy response of aSe to ionizing electrons, and ii) the feasibility to couple a target layer of aSe to a CMOS active pixel sensor to image electron tracks.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Techniques for TPC Calibration: Application to Liquid Ar-TPCs

Large liquid argon TPCs are playing an increasingly important role in neutrino physics, and their calibration will be an essential component of their capability to reach the required performance and precision. Natural sources are extensively used but present limitations, since natural radioactivity from 39 Ar is of low energy, and the rate of cosmic ray muons is low when the detectors are placed deep underground. Argon gas TPCs have been calibrated with ionizing laser beams for several decades, and more recently the technique has been further developed for use in liquid TPCs. Other recent ideas include the use of external neutron generators creating pulses that propagate into the detector. This paper reviews the development of the laser and neutron methods for the calibration of argon TPCs and describes their planned implementation in the upcoming DUNE experiment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS1967

Training course for radiation safety technicians

Course of instruction includes sections on basic information, natural radioactivity, properties of alpha, beta, gamma, X rays, and neutrons, concepts of radiation units and dose determinations, shielding, biological effects, background radiation, radiation protection standards, and internal dose calculation.

Lasuk, S. R.↗
NASA NTRS1972

Gamma-ray spectrometer experiment

The experiments in gamma-ray spectrometry to determine the geochemical composition of the lunar surface are reported. The theory is discussed of discrete energy lines of natural radioactivity, and the lines resulting from the bombardment of the lunar surface by high energy cosmic rays. The gamma-ray spectrometer used in lunar orbit and during transearth coast is described, and a preliminary analysis of the results is presented.

Arnold, J. R.↗
NASA NTRS1973

Expected gamma-ray emission spectra from the lunar surface as a function of chemical composition

The gamma rays emitted from the moon or any similar body carry information on the chemical composition of the surface layer. The elements most easily measured are K, U, Th and major elements such as O, Si, Mg, and Fe. The expected fluxes of gamma ray lines were calculated for four lunar compositions and one chondritic chemistry from a consideration of the important emission mechanisms: natural radioactivity, inelastic scatter, neutron capture, and induced radioactivity. The models used for cosmic ray interactions were those of Reedy and Arnold and Lingenfelter. The areal resolution of the experiment was calculated to be around 70 to 140 km under the conditions of the Apollo 15 and 16 experiments. Finally, a method was described for recovering the chemical information from the observed scintillation spectra obtained in these experiments.

Reedy, R. C.↗