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87 records · Page 5

Titanium-Water Thermosyphon Gamma Radiation Effects and Results

Titanium-water thermosyphons are being considered for use in heat rejection systems for fission power systems. Their proximity to the nuclear reactor will result in some exposure to gamma irradiation. Non-condensable gas formation from radiation may breakdown water over time and render a portion of the thermosyphon condenser inoperable. A series of developmental thermosyphons were operated at nominal operating temperature with accelerated gamma irradiation exposures on the same order of magnitude that is expected in eight years of heat rejection system operation. Temperature data were obtained during exposure at three locations on each thermosyphon; evaporator, condenser, and condenser end cap. Some non-condensable gas was evident, however thermosyphon performance was not affected because the non-condensable gas was compressed into the fill tube region at the top of the thermosyphon, away from the heat rejecting fin. The trend appeared to be an increasing amount of non-condensable gas formation with increasing gamma irradiation dose. Hydrogen is thought to be the most likely candidate for the non-condensable gas and hydrogen is known to diffuse through grain boundaries. Post-exposure evaluation of selected thermosyphons at temperature and in a vacuum chamber revealed that the non-condensable gas likely diffused out of the thermosyphons over a relatively short period of time. Further research shows a number of experimental and theoretical examples of radiolysis occurring through gamma radiation alone in pure water.

Sanzi, James L.↗

A Binary-Encounter-Bethe Approach to Simulate DNA Damage by the Direct Effect

The DNA damage is of crucial importance in the understanding of the effects of ionizing radiation. The main mechanisms of DNA damage are by the direct effect of radiation (e.g. direct ionization) and by indirect effect (e.g. damage by.OH radicals created by the radiolysis of water). Despite years of research in this area, many questions on the formation of DNA damage remains. To refine existing DNA damage models, an approach based on the Binary‐Encounter‐Bethe (BEB) model was developed[1]. This model calculates differential cross sections for ionization of the molecular orbitals of the DNA bases, sugars and phosphates using the electron binding energy, the mean kinetic energy and the occupancy number of the orbital. This cross section has an analytic form which is quite convenient to use and allows the sampling of the energy loss occurring during an ionization event. To simulate the radiation track structure, the code RITRACKS developed at the NASA Johnson Space Center is used[2]. This code calculates all the energy deposition events and the formation of the radiolytic species by the ion and the secondary electrons as well. We have also developed a technique to use the integrated BEB cross section for the bases, sugar and phosphates in the radiation transport code RITRACKS. These techniques should allow the simulation of DNA damage by ionizing radiation, and understanding of the formation of double‐strand breaks caused by clustered damage in different conditions.

Plante, Ianik↗

A Green's Function Approach to Simulate DNA Damage by the Indirect Effect

The DNA damage is of fundamental importance in the understanding of the effects of ionizing radiation. DNA is damaged by the direct effect of radiation (e.g. direct ionization) and by indirect effect (e.g. damage by.OH radicals created by the radiolysis of water). Despite years of research, many questions on the DNA damage by ionizing radiation remains. In the recent years, the Green's functions of the diffusion equation (GFDE) have been used extensively in biochemistry [1], notably to simulate biochemical networks in time and space [2]. In our future work on DNA damage, we wish to use an approach based on the GFDE to refine existing models on the indirect effect of ionizing radiation on DNA. To do so, we will use the code RITRACKS [3] developed at the NASA Johnson Space Center to simulate the radiation track structure and calculate the position of radiolytic species after irradiation. We have also recently developed an efficient Monte‐Carlo sampling algorithm for the GFDE of reversible reactions with an intermediate state [4], which can be modified and adapted to simulate DNA damage by free radicals. To do so, we will use the known reaction rate constants between radicals (OH, eaq, H,...) and the DNA bases, sugars and phosphates and use the sampling algorithms to simulate the diffusion of free radicals and chemical reactions with DNA. These techniques should help the understanding of the contribution of the indirect effect in the formation of DNA damage and double‐strand breaks.

Plante, Ianik↗

A Radiation Chemistry Code Based on the Green's Function of the Diffusion Equation

Stochastic radiation track structure codes are of great interest for space radiation studies and hadron therapy in medicine. These codes are used for a many purposes, notably for microdosimetry and DNA damage studies. In the last two decades, they were also used with the Independent Reaction Times (IRT) method in the simulation of chemical reactions, to calculate the yield of various radiolytic species produced during the radiolysis of water and in chemical dosimeters. Recently, we have developed a Green's function based code to simulate reversible chemical reactions with an intermediate state, which yielded results in excellent agreement with those obtained by using the IRT method. This code was also used to simulate and the interaction of particles with membrane receptors. We are in the process of including this program for use with the Monte‐Carlo track structure code Relativistic Ion Tracks (RITRACKS). This recent addition should greatly expand the capabilities of RITRACKS, notably to simulate DNA damage by both the direct and indirect effect.

Plante, Ianik↗

Pluto: Fluidized Transport of Tholins by Heating of the Subsurface

New Horizons images of Pluto show evidence of the transport of the colored non-ice component across the surface, with substantial accumulations in some areas of low elevation. The non-ice component is presumed to be tholin produced in the atmosphere as a precipitating aerosol, in the surface ices by photolysis or radiolysis, or both. We model the surface layer of N2 ice with varying amounts of incorporated tholin particles to explore the heating within the ice that occurs by the solid-state greenhouse effect. We find that in plausible models of the contaminated N2 surface ice the triple point temperature (63.15K) is reached at a depth of approximately less than 1m. At that depth the confining pressure of the ice column is much less than the triple point pressure (12.52 kPa), so N2 should convert to the gas phase, exerting pressure on the overburden. When the gas pressure exceeds the strength of the confining ice, a breakout on the surface will occur, fluidizing fragments of ice and its contaminants that are then free to flow downhill, rafted on entrained gas, similar in some ways to the pyroclastic volcanic phenomenon known as nuée ardente. The digital elevation map of Pluto made from stereo images shows some surface regions that may have been stripped of the N2 layer, exposing H2O ice (presumed to be bedrock) below, with a corresponding accumulation of dark material that was that was the previously entrained particulate tholin. Accumulations of tholin are found associated with some of the fossae, and some cover preexisting topography to depths of up to a few hundred meters.

New Horizons↗

Oxychlorine Detection in Gale Crater, Mars and Implications for past Environmental Conditions

The Sample Analysis at Mars (SAM) instrument on the Mars Science Laboratory (MSL) rover has detected oxychlorine compounds such as perchlorate or chlorate in Gale Crater samples. Two potential pathways for oxychlorine formation on Mars are UV-induced interaction between chlorine and metal oxides or atmospheric oxygen and radiolysis of Cl-containing surface materials by galactic cosmic rays, with the chlorine being volcanically derived in both cases. Oxychlorine compounds are identified by a diagnostic release of O2 at temperatures <600 °C and an HCl release from ~350-850 °C during sample pyrolysis. Of the 16 samples analyzed by SAM as of July 2018, 12 have contained oxychlorine compounds, including all four scooped samples and 8 of the 12 drilled samples.

Archer, P. Douglas, Jr.↗

Prebiotic Chemistry of Pluto

We present the case for the presence of complex organic molecules, such as amino acids and nucleobases, formed by abiotic processes on the surface and in near-subsurface regions of Pluto. Pluto's surface is tinted with a range of non-ice substances with colors ranging from light yellow to red to dark brown; the colors match those of laboratory organic residues called tholins. Tholins are broadly characterized as complex, macromolecular organic solids consisting of a network of aromatic structures connected by aliphatic bridging units (e.g., Imanaka et al.,2004; Materese et al.,2014, 2015). The synthesis of tholins in planetary atmospheres and in surface ices has been explored in numerous laboratory experiments, and both gas- and solid-phase varieties are found on Pluto. A third variety of tholins, exposed at a site of tectonic surface fracturing called Virgil Fossae, appears to have come from a reservoir in the subsurface. Eruptions of tholin-laden liquid H2O from a subsurface aqueous repository appear to have covered portions of Virgil Fossae and its surroundings with a uniquely colored deposit (D.P. Cruikshank, personal communication) that is geographically correlated with an exposure of H2O ice that includes spectroscopically detected NH3 (C.M. Dalle Ore, personal communication). The subsurface organic material could have been derived from presolar or solar nebula processes, or might have formed in situ. Photolysis and radiolysis of a mixture of ices relevant to Pluto's surface composition (N2, CH4, CO) have produced strongly colored, complex organics with a significant aromatic content having a high degree of nitrogen substitution similar to the aromatic heterocycles pyrimidine and purine (Materese et al.,2014, 2015; Cruikshank et al.,2016). Experiments with pyrimidines and purines frozen in H2O-NH3 ice resulted in the formation of numerous nucleobases, including the biologically relevant guanine, cytosine, adenine, uracil, and thymine (Materese et al.,2017). The red material associated with the H2O ice may contain nucleobases resulting from energetic processing on Pluto's surface or in the interior. Some other Kuiper Belt objects also exhibit red colors similar to those found on Pluto and may therefore carry similar inventories of complex organic materials. The widespread and ubiquitous nature of similarly complex organic materials observed in a variety of astronomical settings drives the need for additional laboratory and modeling efforts to explain the origin and evolution of organic molecules. Pluto observations reveal complex organics on a small body that remains close to its place of origin in the outermost regions of the Solar System.

Cruikshank, D. P.↗

Organic-rich fluids in Pluto’s interior—A source of cryovolcanic activity

The highly variegated surface of Pluto revealed by the New Horizons spacecraft is composed of both volatile ices (N2, CH4, CO) and H2O ice, all of which are intrinsically colorless. The colors on Pluto reveal a non-ice component generally acknowledged to be a refractory complex organic material (tholins) produced by photolysis in the planet’s atmosphere [1], and by photolysis and radiolysis of the surface ices [2-4]. These processes have produced a range of colors from pale yellow to red to brown, and result in a variation of a factor of 10in albedo across the surface. Tholins are disordered polymer-like materials made of repeating chains of linked subunits and complex combinations of functional groups containing carbon. Nitrogen, oxygen, and other elements can be substituted in both the aliphatic and aromatic subunits. The detection of the spectral absorption of an ammoniated compound associated with surface exposures of red-colored H2O ice (herein, RAW) in the LEISA spectral mapping data from New Horizons suggests that a third source of a colored material is ejected from Pluto’s interior as a water-rich fluid(cryomagma) that rapidly freezes at the low temperature (~40K) of the surface [5,6]. The ammoniated compound is thought to be an ammonia hydrate or an ammoniated salt; the spectral data cover a limited wavelength range, resulting in ambiguity in the identification of the form of the ammonia. The distribution of RAW in the vicinity of tectonically stressed and deformed geological structures, particularly graben (fossae), is seen as the result of both fluid effusion and fountaining ejection of cryoclastic materials in Pluto’s Virgil Fossae region [5,6]. RAW is seen elsewhere on Pluto, both in association with graben complexes and on broad expanses of old surface, but primarily in zones of tectonic stress. The nature of the putative subsurface fluid is unknown, but it must have existed at relatively shallow depths such that the graben faulting could reach it. Geochemical modeling of fluids in the interiors of small planetary bodies in the outer Solar System[7] shows that ammonia-bearing H2O in contact with rock and metal components produce a rich chemical soup, including gases that can, in principle, help propel the fluid from shallow reservoirs through crustal fractures to reach the surface. An organic component of the fluid cryomagma is predicted to originate from thermal processing of the components [ref] and may be an example of one-pot synthesis of such complexes as amino acid precursors [ref].

Dale P Cruikshank↗

Radiation-induced D/H Exchange Rate Constants in Aliphatics Embedded in Water Ice

Gas-phase and solid-state chemistry in low-temperature interstellar clouds and cores leads to a D/H enhancement in interstellar ices, which is eventually inherited by comets, meteorites, and even planetary satellites. Hence, the D/H ratio has been widely used as a tracer for the origins of extraterrestrial chemistry. However, the D/H ratio can also be influenced by cosmic rays, which are ubiquitous and can penetrate even dense interstellar molecular cores. The effects of such high-energy radiation on deuterium fractionation have not been studied in a quantitative manner. In this study, we present rate constants for radiation-induced D-to-H exchange for fully deuterated small (1–2 C) hydrocarbons embedded in H2O ice at 20 K and H-to-D exchange for the protiated forms of these molecules in D2O ice at 20 K. We observed larger rate constants for H-to-D exchange in the D2O ice versus D-to-H exchange in H2O ice, which we have attributed to the greater bond strength of C–D versus C–H. We find that the H-to-D exchange rate constants are smaller for protiated methane than ethane, in agreement with bond energies from the literature. We are unable to obtain rate constants for the unsaturated and reactive hydrocarbons ethylene and acetylene. Interpretation of the rate constants suggest that D/H exchange products are formed in abundance alongside radiolysis products. We discuss how our quantitative and qualitative data can be used to interpret the D/H ratios of aliphatic compounds observed throughout space.

Ice destruction↗

Investigating the Impact of X-Ray Computed Tomography Imaging on Soluble Organic Matter in the Murchison Meteorite: Implications for Bennu Sample Analyses

X-ray computed tomography (XCT) is a valuable reconnaissance tool for three-dimensional imaging and identification of distinct lithologies in extraterrestrial samples. It will be used as part of the preliminary examination of samples returned from asteroid (101955) Bennu by the Origins, Spectral Interpretation, Resource Identification, and Security–Regolith Explorer (OSIRIS-REx) mission. However, it must first be established whether x-rays generated during XCT could degrade or alter the organic composition of the returned samples by radiolysis. To test this, we split a crushed sample of the Murchison CM2 meteorite, kept one portion as a control, and irradiated the other portion up to the maximum x-ray dosage (~180 Gy) that a Bennu sample would experience during an XCT imaging experiment. We then extracted organic compounds from both splits and conducted (i) nontargeted soluble organic analyses to compare the chemical distributions of C-, H-, O-, N-, and S-bearing species and (ii) targeted measurements to quantify the abundances of 96 individual soluble organic molecules that included protein amino acids, amines, carboxylic acids, hydroxy acids, carbonyl compounds, polycyclic aromatic hydrocarbons, alcohols, sugars, and N-heterocycles. We found that XCT imaging of the Murchison meteorite had no measurable impact on the relative abundances or enantiomeric compositions of most of the soluble organic compounds targeted in this study. Elevated total abundances of several soluble organic compound classes were observed in the XCT-scanned Murchison sample relative to the control. This is likely related to particle size heterogeneity and specific surface area differences between the sample aliquots used for the extractions, rather than a result of the x-ray exposure. Assuming the samples returned from asteroid Bennu by OSIRIS-REx have a similar composition to carbonaceous chondrites, these data provide confidence that XCT will not significantly alter their soluble organic compositions.

Daniel P Glavin↗

Tracing the Source of Carbon Oxides on the Large Moons of Uranus

The Uranian moons Ariel, Umbriel, Titania, and Oberon are enriched in CO 2 mixed with CO, but the origin(s) of these carbon oxides, be they primarily native or radiolytic, remain(s) uncertain. Using data collected by NIRSpec on the James Webb Space Telescope (JWST), we measured the spectral signature of CO 2 and other carbon oxides to help disentangle these hypotheses. Through comparison to laboratory data, we find that many of the detected spectral features are consistent with CO 2 ice, including 12 CO2 scattering peaks (4.15–4.26 μm), multilobe 13 CO 2 bands (4.35–4.43 μm), and CO 2 biphonon and triphonon modes (4.80–5.25 μm). Our measurements show that CO 2 and CO are concentrated on the trailing hemispheres of the inner moons Ariel and Umbriel, potentially supporting a radiolytic production hypothesis, consistent with prior ground-based results. However, many of the identified spectral features are only observed in thick crystalline ice deposits measured in the laboratory, which may be difficult to form via radiolysis of carbon-bearing material mixed in icy regoliths. Similarly, the data exhibit weak 4.02 and 4.40 μm bands, hinting at the presence of carbonate minerals and 13 CO 2 clathrates, respectively, possibly formed in the interiors of these moons. Furthermore, JWST has revealed that CO 2 is widespread at Uranus, present in its system of rings, ring moons, and irregular satellites, consistent with its largest moons accreting CO 2 and other carbon oxides from the Uranian subnebula. We conclude that exposed carbon oxides are potentially native, with their surface distributions shaped by charged particle irradiation and seasonal sublimation–condensation cycles.

Ice spectroscopy↗

The Radiation Stability of Thymine in Solid H2O

Nucleobases are of significant importance to all known organisms, may be an important building block of life, and could be important biosignatures of current or past life. Given their potential significance to the field of astrobiology, it is important to understand the survival of these molecules when subjected to ionizing radiation as is present in a range of extraterrestrial environments. In this work we present data on the kinetics of the radiolytic destruction of pure thymine, and water + thymine ice mixtures at temperatures from 13 to 150 K. Rate constants were measured using in situ infrared spectroscopy and radiolytic half-lives for thymine were computed for different planetary and interstellar environments. Our results demonstrate that the survival of thymine decreases as the dilution of thymine in water increases. Additionally, we find that thymine survival increases with ice temperature and that this decrease may be related to structure of the ice matrix.

nucleobases, radiolysis, astrobiology↗

Hydrogen Peroxide on the Surface of Europa

Spatially resolved infrared and ultraviolet wavelength spectra of Europa's leading, anti-jovian, quadrant observed from the Galileo spacecraft show absorption features due to hydrogen peroxide.

Jupiter↗

Origin of Molecular Oxygen in Comets: Current Knowledge and Perspectives

The Rosetta Orbiter Spectrometer for Ion and Neutral Analysis (ROSINA) instrument onboard the Rosetta spacecraft has measured molecular oxygen (O 2 ) in the coma of comet 67P/Churyumov-Gerasimenko (67P/C-G) in surprisingly high abundances. These measurements mark the first unequivocal detection of O 2 in a cometary environment. The large relative abundance of O 2 in 67P/C-G despite its high reactivity and low interstellar abundance poses a puzzle for its origin in comet 67P/C-G, and potentially other comets. Since its detection, there have been a number of hypotheses put forward to explain the production and origin of O 2 in the comet. These hypotheses cover a wide range of possibilities from various in situ production mechanisms to protosolar nebula and primordial origins. Here, we review the O2 formation mechanisms from the literature, and provide a comprehensive summary of the current state of knowledge of the sources and origin of cometary O 2 .

Molecular oxygen↗