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At least 847 records · Page 47
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Dioctyl ether radiolysis under used nuclear fuel reprocessing conditions: Foundational knowledge for the development of sacrificial ligand grafts

Radiation-induced ligand destruction and concomitant degradation product formation is unavoidable under envisioned used nuclear fuel reprocessing conditions, and ultimately limits the recyclability of a given solvent system formulation. With this in mind, a novel approach to ligand innovation for advanced separations processes is in the design of tailored “protomolecules,” which when exposed to ionizing radiation undergo desired chemical transformations, thereby allowing for a reprocessing solvent system to advantageously evolve with absorbed radiation dose. Here we provide foundational knowledge for the time-resolved (electron pulse) and steady-state (cobalt-60 gamma) radiolytic behavior of dioctyl ether, a protomolecule grafting surrogate. Gamma irradiation of single-phase solutions of dioctyl ether (5–100 vol.%) in n-dodecane resulted in the loss of dioctyl ether (G = -0.72 µmol J –1 ) and the formation of octane (G = 0.11 µmol J –1 ) and octanol (G = 0.15 µmol J –1 ) degradation products, the latter of which is a known reprocessing phase modifier and radioprotectant. Further, these radiation-induced changes were attributed to direct radiation effects, for more concentrated dioctyl ether solutions, and indirect radiation effects, predominantly driven by the reaction of dioctyl ether with the dodecane radical cation, for which we report a second-order rate coefficient of k = (1.53 ± 0.05) × 10 10 L mol –1 s –1 . Under typical biphasic extraction (4.0 mol L –1 HNO 3 ) and strip (0.1 mol L –1 HNO 3 ) reprocessing conditions, gamma irradiation of 5 vol.% dioctyl ether solvent systems afforded negligible change in the rate of parent molecule destruction but promoted significant differences in the radiolytic behavior of its degradation products. These differences are attributed to their respective interactions with [dioctyl ether/HNO 3 /H 2 O] and [octanol/HNO 3 /H 2 O] adducts extracted into the organic phase. Overall, these results support the grafting of ether linkages to advanced separations ligands (e.g., modified diglycolamides).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS1993

Micromachined Electron-Tunneling Infrared Detectors

Pneumatic/thermal infrared detectors based partly on Golay-cell concept, but smaller and less fragile. Include containers filled with air or other gas trapped behind diaphragms. Infrared radiation heats sensors, causing gas to expand. Resulting deflections of diaphragms measured by displacement sensors based on principle of electron-tunneling transducers of scanning tunneling microscopes. Exceed sensitivity of all other miniature, uncooled infrared sensors presently available. Expected to include low consumption of power, broadband sensitivity, room-temperature operation, and invulnerability to ionizing radiation.

Kenny, Thomas W.↗
NASA NTRS1992

Seyfert galaxy ultraviolet emission-line intensities and variability - A self-consistent photoionization analysis applied to broad-line-emitting gas in NGC 3783

Well-constrained photoionization models for the Seyfert I galaxy NGC 3783 are developed. Both cross-correlation analyses and line variability trends with varying ionizing radiation flux require a multicomponent picture. All the data for He II 1640 A, C IV 1549 A, and semiforbidden C III 1909 A can be reasonably well reproduced by two cloud components. One has a source-cloud distance of 24 lt-days, gas density around 3 x 10 exp 10/cu cm, ionization parameter range of 0.04-0.2, and cloud thickness such that about half of the carbon is doubly ionized and about half is triply ionized. The other component is located approximately 96 lt-days from the source, is shielded from the source by the inner cloud, has a density about 3 x 10 to the 9th/cu cm, and is characterized by an ionization parameter range of 0.001-0.03, The cloud thickness is such that about 45 percent carbon is doubly ionized and about 55 percent is singly ionized.

Koratkar, Anuradha P.↗
NASA NTRS1994

Composition of interstellar clouds in the disk and halo. 2: Gamma(sup 2) Velorum

High-resolution observations of gamma(sup 2) Vel with the Goddard High-Resolution Spectrograph (GHRS) echelle on the Hubble Space Telescope reveal the presence of seven narrow absorption components, with LSR velocities between -23 and +9 km s(exp -1). Three of these show column density ratios N(S(++))/N(S(+)) and N(P(++))/N(P+)) of about 1 or more, and can be identified as H II regions, while the other four are H I regions, consistent with the O I profile and with the overall H(sup 0) column density of 5.9 x 10(exp 19) cm(exp -2), given the usual assumptions that S is undepleted while O has a depletion D(O) = -0.3 dex. The depletions of Fe, Si, and Mn, which could be measure accurately for two of the four H I regions (components 6 and 7), differ somewhat from the values of D(sub ws) found for slowly moving warm clouds in HD 93521; in particular, for the component at 4.0 km s(exp -1) (No. 6), abosolute of D exceeds absolute of D(sub ws) by 0.1-0.4 dex, while for that at 9.3 km s(exp -1) (No. 7), absolute of D equals absolute of D(sub ws) on the average. The observed ratio of Fe + Mg atoms to Si atoms in the grains of component 6 is 2.04 +/-0.10, consistent with an olivine grain composition; the Fe/Mg ratio is 1.5 +/- 0.2. The electron density in component 6, determined from the C II(sup *) feature, is 0.075 +/- 0.013 cm (exp -3), about two-thirds of that found for clouds of this velocity in HD 93521. In the two conspicuous H II regions, components 3 and 4, n(sub e), determined from the Si II(sup *) feature, is about 1 cm(exp -3). From the column density of S(+) + S(++) in these two components, the total H II path length is about 40 pc. With the radius of a wind-blown bubble around gamma(sup 2) Vel set equal to 60 pc, the effective Stromgren radius is about 100 pc, requiring that T approx. equal to 50,000 K for the Wolf-Rayet component of the gamma(sup 2) Vel binary. Since zeta Pup is a comparable source of ionizing radiation, this temperature is an upper limit. The profiles of the strongest H2 absorption features, from Copernicus archives, indicate that the absorbing molecules have a mean velocity identical with that of the strongest H II component (No. 4). We have no explanation for the possible presence of these H2 molecules in a region of ionized H. Alternatively, the H2 profiles can be explained by molecules in the two adjacent (in velocity) H I regions, components 2 and 5, provided their H I gas has densities and temperatures typical of normal cold clouds. The GHRS data show absorption by highly ionized atoms Si(3+) and C(3+), N(4+) in broad features, in addition to the narrow-line absorption by Si(3+) and C(3+) observed in the dominant H II components, Nos. 3 and 4. The broad C(3+) and N(4+) features have widths corresponding to T in the range (4-8) x 10(exp 5) K, consistent with the broad O(5+) line shown in Copernicus data. Despite some observational uncertainties, the ratios of column densities in the broad C(3+), N(4+), and O(5+) features agree to +/- 0.1 dex with theoretical values for warm gas, heating and evaporating by thermal conduction from an adjacent hot region. Outward evaporation from an isolated cloud in a hot ambient gas cannot be distinguished, on the basis of these data, from inward evaporation of a warm shell, compressed by an expanding, hot stellar-wind bubble. For several halo stars, the C IV/O VI ratio has a quite different average value, perhaps consistent with cooling of infalling hot gas instead of conductive heating and evaporation.

Fitzpatrick, Edward L.↗
DOE OSTI2023

Actinide Radiation Chemistry and Used Nuclear Fuel Reprocessing

Although the actinides boast many unique physical and chemical properties, their inherent susceptibility to radioactive decay—and subsequent consequences of radiation-induced chemistry—are what make them truly interesting and challenging elements to understand. From a closed nuclear fuel cycle perspective, the ability to predict and control the effects of actinide-driven radiolysis is critical for the design, development, and deployment of advanced used nuclear fuel reprocessing strategies and technologies. The absorption of ionizing radiation from actinide decay leads to the formation of a variety of transient and steady-state radicals, ions, and molecular radiolysis products that can lead to significant changes in a reprocessing solvent system’s physical and chemical properties, which ultimately limits that process’ efficiency and longevity. Presented here is an overview of recent advances in actinide radiation chemistry as it applied to used nuclear fuel reprocessing.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS1989

Late cataractogenesis caused by particulate radiations and photons in long-lived mammalian species

Radiation cataractogenesis induced by small acute doses of particulate radiations and photons in the New Zealand white rabbit (Oryctolagus cuniculus), the beagle dog (Canis familiaris) and the rhesus monkey (Macaca mulatta) is discussed in the context of the use of animal models to assess the radiation hazards faced by humans during lengthy sojourns in deep space. Attention is paid to (1) the importance of lifespan studies with long-lived species - the above animals have median lifespans in captivity of 5-7, 13-14 and 25 years, respectively; and (2) the magnitudes of possible dose thresholds for cataractogenesis from sparsely ionizing radiations and the modifications of those thresholds by the late degenerative phase of the phenomenon.

Lett, J. T.↗
NASA NTRS1992

Damage to cellular DNA from particulate radiations, the efficacy of its processing and the radiosensitivity of mammalian cells. Emphasis on DNA double strand breaks and chromatin breaks

For several years, it has been evident that cellular radiation biology is in a necessary period of consolidation and transition (Lett 1987, 1990; Lett et al. 1986, 1987). Both changes are moving apace, and have been stimulated by studies with heavy charged particles. From the standpoint of radiation chemistry, there is now a consensus of opinion that the DNA hydration shell must be distinguished from bulk water in the cell nucleus and treated as an integral part of DNA (chromatin) (Lett 1987). Concomitantly, sentiment is strengthening for the abandonment of the classical notions of "direct" and "indirect" action (Fielden and O'Neill 1991; O'Neill 1991; O'Neill et al. 1991; Schulte-Frohlinde and Bothe 1991 and references therein). A layer of water molecules outside, or in the outer edge of, the DNA (chromatin) hydration shell influences cellular radiosensitivity in ways not fully understood. Charge and energy transfer processes facilitated by, or involving, DNA hydration must be considered in rigorous theories of radiation action on cells. The induction and processing of double stand breaks (DSBs) in DNA (chromatin) seem to be the predominant determinants of the radiotoxicity of normally radioresistant mammalian cells, the survival curves of which reflect the patterns of damage induced and the damage present after processing ceases, and can be modelled in formal terms by the use of reaction (enzyme) kinetics. Incongruities such as sublethal damage are neither scientifically sound nor relevant to cellular radiation biology (Calkins 1991; Lett 1990; Lett et al. 1987a). Increases in linear energy transfer (LET infinity) up to 100-200 keV micron-1 cause increases in the extents of neighboring chemical and physical damage in DNA denoted by the general term DSB. Those changes are accompanied by decreasing abilities of cells normally radioresistant to sparsely ionizing radiations to process DSBs in DNA and chromatin and to recover from radiation exposure, so they make significant contributions to the relative biological effectiveness (RBE) of a given radiation.(ABSTRACT TRUNCATED AT 400 WORDS).

Non-NASA Center↗
NASA NTRS2009

Extraterrestrial Radiation Chemistry and Molecular Astronomy

Astronomical observations of both solar system and interstellar regions have revealed a rich chemical inventory that includes most classes of organic molecules and selected inorganics. For example, gas-phase ethylene glycol and SOz have been observed by astronomers, while solidphase detections include OCS, H2O2 , and the cyanate anion.' All of these are found in environments that are, by earthly standards, exceedingly hostile: temperatures of 10 - 100 K, miniscule densities, and near-ubiquitous ionizing-radiation fields. Beyond the simplest chemical species, these conditions have made it difficult-to-impassible to account for the observed molecular abundances using gas-phase chemistry, suggesting solid-phase reactions play an important role. In extraterrestrial environments, cosmic rays, UV photons, and magnetospheric radiation all drive chemical reactions, even at cryogenic temperatures. To study this chemistry, radiation astrochemists conduct experiments on icy materials, frozen under vacuum and exposed to sources such as keV electrons and MeV protons. Compositional changes usually are followed with IR spectroscopy and, in selected cases, more-sensitive mass-spectral techniques. This talk will review some recent results on known and suspected extraterrestrial molecules and ions. Spectra and reaction pathways will be presented, and predictions made for interstellar chemistry and the chemistry of selected solar system objects. Some past radiation-chemical contributions, and future needs, will be explored.

Hudson, Reggie L.↗
NASA NTRS2002

The action of a dietary retinoid on gene expression and cancer induction in electron-irradiated rat skin

Current models of radiation carcinogenesis generally assume that the DNA is damaged in a variety of ways by the radiation and that subsequent cell divisions contribute to the conversion of the damage to heritable mutations. Cancer may seem complex and intractable, but its complexity provides multiple opportunities for preventive interventions. Mitotic inhibitors are among the strongest cancer preventive agents, not only slowing the growth rate of preneoplasias but also increasing the fidelity of DNA repair processes. Ionizing radiation, including electrons, is a strong inducer of cancer in rat skin, and dietary retinoids have shown potent cancer preventive activity in the same system. A non-toxic dietary dose of retinyl acetate altered gene expression levels 24 hours after electron irradiation of rat skin. Of the 8740 genes on an Affymetrix rat expression array, the radiation significantly (5 fold or higher) altered 188, while the retinoid altered 231, including 16 radiation-altered genes that were reversely altered. While radiation strongly affected the expression of stress response, immune/inflammation and nucleic acid metabolism genes, the retinoid most strongly affected proliferation-related genes, including some significant reversals, such as, keratin 14, retinol binding protein, and calcium binding proteins. These results point to reversal of proliferation-relevant genes as a likely basis for the anti-radiogenic effects of dietary retinyl acetate.

Non-NASA Center↗
DOE OSTI2025

Modeling of surface-state induced inter-electrode isolation of n -on- p devices in mixed-field and γ -irradiation environments

Position sensitive n-on-p silicon sensors will be utilized in the tracker and in the High Granularity Calorimeter (HGCAL) of the Compact Muon Solenoid (CMS) experiment at High Luminosity Large Hadron Collider (HL-LHC). The detrimental effect of the radiation-induced accumulation of positive net oxide charge on position resolution in n-on-p sensors has typically been countered by the application of isolation implants like p-stop or p-spray between n + -electrodes. In addition to the positively charged layer inside the oxide and close to the Si/SiO 2 -interface, surface damage introduced by ionizing radiation in SiO 2 -passivated silicon particle detectors includes the accumulation of trapped-oxide-charge and interface traps. A previous study of either n/γ (mixed field)- or γ-irradiated Metal-Oxide-Semiconductor (MOS) capacitors showed evidence of substantially higher introduction rates of acceptor- and donor-type deep interface traps (N it,acc/don ) in mixed-field environment. Here, in this work, an inter-pad and -strip resistance (or resistivity (ρ int )) simulation study of n-on-p sensors with and without p-stop isolation implants was conducted for both irradiation types. Higher levels of ρint showed correlation to higher densities of deep N it,acc/don , with the inter-pad isolation performance of the mixed-field irradiated sensors becoming independent of the presence of p-stop implant between the n + - electrodes up to about 100 kGy. The low introduction rates of deep N it,acc/don in γ-irradiated sensors resulted in high sensitivity of ρ int to the presence and peak doping of p-stop above the lowest dose of about 7 kGy in the study. As a consequence of the advantageous influence of radiation-induced accumulation of deep N it on the inter-electrode isolation, position sensitive n-on-p sensors without isolation implants may be considered for future HEP-experiments where the radiation is largely due to hadrons.

Akchurin, N. [Texas Tech Univ., Lubbock, TX (Unite↗
NASA NTRS1992

The ionosphere as a gamma ray burst detector

Unlike all man made detectors, which are only sensitive to relative narrow regions of the electromagnetic spectrum, the ionosphere is practically a perfect detector for high energy radiation because it absorbs all radiation from the far-ultraviolet to the higher energy gamma-rays. Therefore, it may be possible to employ the terrestrial atmosphere as a detector of high energy celestial photons. As early as the 1940's solar flares were detected by the disturbance they caused to the ionosphere. The VLF (3 - 30 kHz) approach for detecting ionospheric disturbances is based on the following physical circumstance: celestial high energy radiation ionizes the atoms of the earth's ionosphere leading to the production of free electrons. These free electrons influence the propagation of electromagnetic waves. By studying the phase and amplitude changes of VLF radio wave propagating in the earth-ionosphere waveguide, it was hoped to ascertain the electron density in these regions and draw conclusions about the celestial radiation which caused them. To detect gamma-ray bursts, two conditions for the optimal detection are: (1) large zenith angle; and (2) alignment of burst and propagation path.

Mcgruder, Charles H., III↗
NASA NTRS2003

Switching Oxide Traps

We consider radiation-induced charge trapping in SiO2 dielectric layers, primarily from the point of view of CMOS devices. However, SiO2 insulators are used in many other ways, and the same defects occur in other contexts. The key studies, which determined the nature of the oxide charge traps, were done primarily on gate oxides in CMOS devices, because that was the main radiation problem in CMOS at one time. There are two major reviews of radiation-induced oxide charge trapping already in the literature, which discuss the subject in far greater detail than is possible here. The first of these was by McLean et al. in 1989, and the second, ten years later, was intended as an update, because of additional, new work that had been reported. Basically, the picture that has emerged is that ionizing radiation creates electron-hole pairs in the oxide, and the electrons have much higher mobility than the holes. Therefore, the electrons are swept out of the oxide very rapidly by any field that is present, leaving behind any holes that escape the initial recombination process. These holes then undergo a polaron hopping transport toward the Si/SiO2 interface (under positive bias). Near the interface, some fraction of them fall into deep, relatively stable, long-lived hole traps. The nature and annealing behavior of these hole traps is the main focus of this paper.

Oldham, Timothy R.↗
NASA NTRS1992

Absorbed dose measurements and predictions on LDEF

The overall radiation environment of LDEF was determined in part through the use of thermoluminescent detectors (TLDs). The results given are from four experiments (Biostack, Fiber Optics Data Link, Seeds in Space, and Linear Energy Transfer Spectrum Measurement) and represent a large fraction of existing absorbed dose data. The TLDs (located on leading and trailing edges) were under various shielding depths. The measured absorbed doses were found to reflect both directional dependence of incident trapped protons and shielding. Radiation dosages at both locations and under various shielding depths are given. The effect of the trapped proton anisotropy was such that the western side of LDEF received about 3 times the dose of the eastern side at shielding depths of approx. 1 gm/sq cm. These data are being used to evaluate the accuracy of models currently in use for predicting ionizing radiation environments for low Earth orbit missions.

Frank, A. L.↗
DOE OSTI2022

Investigation of the Solution Chemistry of Hybrid Organic–Inorganic Indium Halides for New Material Discovery

Recently, metal halide perovskites (MHPs) have emerged as a new class of materials for optical and electronic applications such as solar cells and ionizing radiation detectors. Although the solution-processability of MHPs is among their greatest advantages, the solution chemistries of most metal halide systems and their relationship with the observed structural and chemical diversity are poorly understood. In this work, we study the solution chemistry of a model indium halide system, methylammonium (MA)–In–Br, using a combination of the UV–vis spectroscopy, electrospray ionization mass spectrometry (ESI-MS) measurements, small-angle X-ray scattering (SAXS), and density functional theory (DFT) calculations. Our results show that indium could form either octahedral [InBr 6 3– ] or tetrahedral [InBr 4 – ] anions in solution or a combination of both, depending on the loading ratios of MABr and InBr 3 reactants. Understanding the solution chemistry of this system and recognizing the optical fingerprints of these polyanions allow for targeted crystallization of two novel compounds: MAInBr 4 featuring tetrahedral [InBr 4 – ] anions and MA 2 InBr 5 containing both octahedral [InBr 6 3– ] and tetrahedral [InBr 4 – ] anions. Further increase of the MABr content leads to the formation of previously reported MA 4 InBr 7 , containing only octahedral [InBr 6 3– ] anions separated by Br – anions. Furthermore, our results suggest that understanding the solution chemistry of multinary metal halide systems could be a valuable tool for discovering functional materials for practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2001

Cell and Molecular Biology of Ataxia Telangiectasia Heterozygous Human Mammary Epithelial Cells Irradiated in Culture

Autologous isolates of cell types from obligate heterozygotes with the autosomal disorder ataxia-telangiectasia (A-T)were used to begin a tissue culture model for assessing pathways of radiation-induced cancer formation in this target tissue. This was done by establishing cultures of stromal fibroblasts and long-term growth human mammary epithelial cells (HMEC) in standard 2-dimensional tissue culture in order to establish expression of markers detailing early steps of carcinogenesis. The presumptive breast cancer susceptibility of A-T heterozygotes as a sequel to damage caused by ionizing radiation provided reason to study expression of markers in irradiated HMEC. Findings from our study with HMEC have included determination of differences in specific protein expression amongst growth phase (e.g., log vs stationary) and growth progression (e.g., pass 7 vs pass 9), as well as differences in morphologic markers within populations of irradiated HMEC (e.g., development of multinucleated cells).

Richmond, Robert C.↗
NASA NTRS2005

Human Exploration of the Moon and Mars: Space Radiation Data, Modeling and Instrumentation Needs

On January 14, 2004 President Bush announced the Vision for Space Exploration, a program for long-term human and robotic exploration of the solar system which will include a return of humans to the moon not later than 2020, followed by human missions to Mars. Since this announcement, NASA has been developing plans and mission architectures for these human missions as well as robotic precursor missions. Among the critical needs for research and development in support of this Vision are investigations on the ionizing radiation environment and development of instrumentation to guide NASA in managing the radiation exposure of the crew during the manned missions. For mission planning, models are needed for a reference worst-case solar energetic particle event and a reference worst-case galactic cosmic ray environment. During Lunar missions it will be necessary to carefully manage the radiation exposure of the crew in real time because of the variability of the radiation environment due to solar activity. In particular, prompt warnings will be needed when large solar energetic particle events occur. Accurate predictions will also be needed of the particle flux and flux history at the moon to support critical mission management decisions. A new generation of dosimeters and radiation monitors will also be needed to accompany the crew. These instruments must return data in real time so that they can be used in the critical decisions that must be made if a large solar energetic particle event occurs. This is especially true if it occurs during a lunar excursion. A substantial radiation exposure on extended lunar missions and Mars missions comes from galactic cosmic rays. This exposure must be mitigated by radiation shielding and other measures. During Mars missions the galactic cosmic ray exposure occurs primarily during the cruse phase between the Earth and Mars. This is especially true for opposition class missions. These missions would typically last -430 days with only 30-90 days on Mars. Solar energetic particle events are less of a concern on Mars because of its greater distance from the Sun (approximately 1.5 AU) and the partial protection afforded by its atmosphere (approximately 20 grams per square centimeter). The talk will describe the current plans for future human missions to Earth orbit, the Moon and Mars. The needs for data and models of the radiation environment and radiation detectors to support these missions will be discussed.

Adams, James H.↗
DOE OSTI2024

Cutaneous Radiation Injuries: REAC/TS Clinical Experience

Abstract The Radiation Emergency Assistance Center/Training Site (REAC/TS) is one of the US Department of Energy (DOE)/National Nuclear Security Administration (NNSA) Nuclear Emergency Response Team (NEST) assets and has been responding to radiological incidents since 1976. REAC/TS is in the Oak Ridge Institute for Science and Education (ORISE). A critical part of the REAC/TS mission is to provide emergency response, advice, and consultation on injuries and illnesses caused from ionizing radiation. Fortunately, radiation injuries are not frequent, but when they occur, they are more likely to be cutaneous radiation injuries (CRI) or internal contamination. In this paper, we will review selected cases from the REAC/TS experience in order to illustrate cutaneous patterns of injury and treatment options.

Public, Environmental & Occupational Health↗
NASA NTRS1990

What produces the ionizing background at large redshift?

Results are presented from mathematical and modeling studies to make estimates of the intensity of the ionizing background more definite and quantitative. It is shown that the observed quasars fail to emit sufficient ionizing radiation to satisfy the Gunn-Peterson test. Two possible sources for the additional source of UV radiation are examined: main-sequence, high mass stars in primordial galaxies and quasars that have not been observed because of dust obscuration. Both of these models satisfy the observational constraints with reasonable parameters. It is suggested that observations of He lines from Ly-alpha clouds or an analysis of the line ratios in metal line absorption systems may be used to determine which sources produce the ionizing background.

Miralda-Escude, Jordi↗