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At least 19 records

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NASA NTRS1982

Time-resolved spectroscopy of solid poly/1-vinyl naphthalene/ following electron beam pulse radiolysis - Pulse radiolytic studies on polymers

Transient emission studies following pulse radiolysis of solid poly(1-vinyl naphthalene) show existence of excited monomers and two excimers. Quenching experiments indicate that excimers are not formed directly by recombination of ions but probably by trapping of migrating monomeric excitation in preformed traps whose density is approximately one in 1000.

Coulter, D. R.↗

NASA NTRS2006

Volume Ice Radiolysis in the Outer Solar System

The primary energy flux of charged particle components of the heliospheric and magnetospheric environments of the solar system is primarily carried by highly penetrating energetic particles. Although laboratory experiments on production of organics and oxidants typically only address effects on very thin surface layers, energy deposition occurs on surfaces of icy bodies of the outer solar system to meters in depth. Time scales for significant radiolytic deposition vary from thousands of years at millimeter depths on Europa to billions of years in the meters-deep regolith of Kuiper Belt Objects. Radioisotope decay (e.g., K-40) also contributes to volume radiolysis as the only energy source at much greater depths. Radiolytic oxygen is a potential resource for life within Europa and a partial source of oxygen for Saturn's magnetosphere and Titan's upper atmosphere. Interactions of very high energy cosmic rays with ices at Titan's surface may provide one of the few sources of oxidants in that highly reducing environment. The red colors of low-inclination classical Kuiper Belt Objects at 40-50 AU, and Centaur objects originating from this same population, may arise from volume radiolysis of deep ice layers below more refractory radiation crusts eroded away by surface sputtering and micrometeoroid impacts. A variety of techniques are potentially available to measure volume radiolysis products and have been proposed for study as part of the new Space Physics of Life initiative at NASA Goddard Space Flight Center. The technique of Electron Paramagnetic Resonance (EPR) has been used in medical studies to measure oxidant production in irradiated human tissue for cancer treatment. Other potential techniques include optical absorption spectroscopy and standard wet chemical analysis. These and other potential techniques are briefly reviewed for applicability to problems in solar system ice radiolysis and astrobiology.

Cooper, John F.↗

NASA NTRS1982

Pulsed radiolysis of model aromatic polymers and epoxy based matrix materials

Models of primary processes leading to deactivation of energy deposited by a pulse of high energy electrons were derived for epoxy matrix materials and polyl-vinyl naphthalene. The basic conclusion is that recombination of initially formed charged states is complete within 1 nanosecond, and subsequent degradation chemistry is controlled by the reactivity of these excited states. Excited states in both systems form complexes with ground state molecules. These excimers or exciplexes have their characteristics emissive and absorptive properties and may decay to form separated pairs of ground state molecules, cross over to the triplet manifold or emit fluorescence. ESR studies and chemical analyses subsequent to pulse radiolysis were performed in order to estimate bond cleavage probabilities and net reaction rates. The energy deactivation models which were proposed to interpret these data have led to the development of radiation stabilization criteria for these systems.

Gupta, A.↗

NASA NTRS2017

Coloring Jupiter's Clouds: Radiolysis of Ammonium Hydrosulfide (NH4SH)

Here we present our recent studies on the color and spectral reflectance changes induced by approximately 0.9 megaelectronvolts proton irradiation of ammonium hydrosulfide, NH4SH, a compound predicted to be an important tropospheric cloud component of Jupiter and other giant planets. Ultraviolet-visible spectroscopy was used to observe and identify reaction products in the ice sample and digital photography was used to document the corresponding color changes at 10-160 degrees Kelvin. Our experiments clearly show that the resulting color of the sample depends not only on the irradiation dose but also the irradiation temperature. Furthermore, unlike in our most recent studies of irradiation of NH4SH at 120 degrees Kelvin, which showed that higher irradiation doses caused the sample to appear green, the lower temperature studies now show that the sample becomes red after irradiation. However, comparison of these lower temperature spectra over the entire spectral range observed by HST (Hubble Space Telescope) shows that even though the color and spectrum resemble the color and spectrum of the GRS (Jupiter’s Great Red Spot), there is still enough difference to suggest that another component may be needed to adequately fit spectra of the GRS and other red regions of Jupiter's clouds. Regardless, the presence of NH4SH in the atmosphere of Jupiter and other gas giants, combined with this compound's clear alteration via radiolysis, suggests that its contribution to the ultraviolet-visible spectra of any of these object's clouds is significant.

ultraviolet-visible spectroscopy↗

NASA NTRS2012

In-situ Measurements of the Radiolytic Destruction of Glycine in Ices: Applications to the Martian Subsurface

Amino acids and other organic molecules are thought to be easily destroyed on the surface of Mars by the high flux of incident ultraviolet rays or by chemical interactions with oxidizing substances in the soil. However, organic molecules may survive in the subsurface, where chemical processes are driven by penetrating galactic cosmic rays such as MeV protons. Models of the radiation dose as a function of depth on Mars have shown that the contribution of galactic cosmic rays dominates from about one centimeter to a few meters [1 J. Theoretical models have also been published to aid in understanding molecular destruction at these depths, but these usually are based on room-temperature laboratory data, studies of single-component samples, and ex-situ methods of chemical analysis. Recent studies of amino-acid survivability include those involving UV photolysis [2, 3J and gamma radiolysis [4], but nearly all chemical and kinetic analyses from such experiments involved room-temperature measurements on samples irradiated and then removed from sealed containers. We report new laboratory studies of the radiation-induced destruction of glycine-containing ices. In-situ infrared spectroscopy was used to study decay rates as a function of temperature and initial glycine concentrations. Our results indicate that glycine's destruction rate depends on temperature, the presence of H20-ice, and the initial relative abundance of glycine. These trends are not obvious in previous work, suggesting that room-temperature measurements on pure glycine's radiation stability are not directly applicable to Mars and other environments.

Gerakines, Perry A.↗

NASA NTRS2012

New Modeling Approaches to Study DNA Damage by the Direct and Indirect Effects of Ionizing Radiation

DNA is damaged both by the direct and indirect effects of radiation. In the direct effect, the DNA itself is ionized, whereas the indirect effect involves the radiolysis of the water molecules surrounding the DNA and the subsequent reaction of the DNA with radical products. While this problem has been studied for many years, many unknowns still exist. To study this problem, we have developed the computer code RITRACKS [1], which simulates the radiation track structure for heavy ions and electrons, calculating all energy deposition events and the coordinates of all species produced by the water radiolysis. In this work, we plan to simulate DNA damage by using the crystal structure of a nucleosome and calculations performed by RITRACKS. The energy deposition events are used to calculate the dose deposited in nanovolumes [2] and therefore can be used to simulate the direct effect of the radiation. Using the positions of the radiolytic species with a radiation chemistry code [3] it will be possible to simulate DNA damage by indirect effect. The simulation results can be compared with results from previous calculations such as the frequencies of simple and complex strand breaks [4] and with newer experimental data using surrogate markers of DNA double ]strand breaks such as . ]H2AX foci [5].

Plante, Ianik↗

NASA NTRS2024

Organic Products of Fatty Acid and Magnesium Sulfate Mixtures after Gamma Radiolysis: Implications for Missions to Europa

If ocean-derived materials are present at Europa’s surface, they would represent accessible records of ocean chemistry and habitability, but such materials would be further processed by the moon’s harsh radiation environment. In this study, saturated fatty acids were precipitated onto a Europa-relevant hydrated magnesium sulfate and exposed to gamma radiation doses up to 2 MGy at -196° C. Alkane chains, with carbon numbers one less than those of the starting fatty acids, were the most abundant radiolysis products in solvent and thermal extracts analyzed by gas chromatography mass spectrometry. Detections of monounsaturated fatty acids and combined radiolysis products were attributed to the experiment’s Europa-like parameters. Additionally, elevated concentrations of shorter-chain saturated fatty acids suggest that gamma radiation induced charge remote fragmentation of the alkyl chains of some starting fatty acids under these experimental conditions. Quantitation of fatty acid concentrations in the irradiated samples enabled the calculation of a radiolysis constant that indicated exposure to a 5 MGy dose of gamma radiation would have resulted in a ~90% loss of the initial fatty acid population. The samples were further studied by Raman spectroscopy and laser desorption and ionization mass spectrometry, which characterized the distribution of fatty acids and their radiolysis products on sulfate surfaces. The substantial loss of starting fatty acids typically seen with increasing radiation dose, along with the remarkable diversity of radiolysis products identified, suggest that the detection of fatty acids in irradiated sulfate deposits on Europa will be challenged by rapid destruction of any initial fatty acid populations and scrambling of their residual signals by a myriad of organic radiolysis products. If missions to Europa encounter sulfate deposits, targeting minimally irradiated units may still enable the detection of surviving fatty acid signatures that could inform about Europa’s subsurface chemistry and habitability.

James M T Lewis↗

NASA NTRS2011

Radiolysis of Sulfuric Acid, Sulfuric Acid Monohydrate, and Sulfuric Acid Tetrahydrate and Its Relevance to Europa

We report laboratory studies on the 0.8 MeV proton irradiation of ices composed of sulfuric acid (H2SO4), sulfuric acid monohydrate (H2SO4 H2O), and sulfuric acid tetrahydrate (H2SO4 4H2O) between 10 and 180 K. Using infrared spectroscopy, we identify the main radiation products as H2O, SO2, (S2O3)x, H3O+, HSO4(exp -), and SO4(exp 2-). At high radiation doses, we find that H2SO4 molecules are destroyed completely and that H2SO4 H2O is formed on subsequent warming. This hydrate is significantly more stable to radiolytic destruction than pure H2SO4, falling to an equilibrium relative abundance of 50% of its original value on prolonged irradiation. Unlike either pure H2SO4 or H2SO4 H2O, the loss of H2SO4 4H2O exhibits a strong temperature dependence, as the tetrahydrate is essentially unchanged at the highest irradiation temperatures and completely destroyed at the lowest ones, which we speculate is due to a combination of radiolytic destruction and amorphization. Furthermore, at the lower temperatures it is clear that irradiation causes the tetrahydrate spectrum to transition to one that closely resembles the monohydrate spectrum. Extrapolating our results to Europa s surface, we speculate that the variations in SO2 concentrations observed in the chaotic terrains are a result of radiation processing of lower hydration states of sulfuric acid and that the monohydrate will remain stable on the surface over geological times, while the tetrahydrate will remain stable in the warmer regions but be destroyed in the colder regions, unless it can be reformed by other processes, such as thermal reactions induced by diurnal cycling.

Loeffler, M. J.↗

NASA NTRS1979

An analytical approach to evaluation of space radiation effects on materials for long-life missions

An analytical model was developed which quantifies effects on organic composite matrix materials of high energy electrons and of UV as well as interactions between the two radiations. Literature data on polyethylene were used to construct a degradation kinetics scheme corresponding to an Earth orbit at L=3. Analysis of the model showed that steady state concentrations of radicals put limits on accelerated test conditions. These conclusions were validated by an experimental study on polymethylmethacrylate using UV laser excitation. Relationships for balancing electron and UV radiations to equal acceleration factors are derived. Pulse radiolysis using an electron-beam along with time-resolved spectroscopy is shown to be able to separate primary form secondary reactions. Implications of these reactions to changes in engineering material properties are indicated. The use of mechanistic studies is discussed in the context of general test strategies for evaluating materials for space applications.

Moacanin, J.↗

NASA NTRS2019

Radiolysis of Macromolecular Organic Material in Mars-Relevant Mineral Matrices

The fate of organic material on Mars after deposition is crucial to interpreting the source of these molecules. Previous work has addressed how various organic compounds at millimeter depths in sediments respond to ultraviolet radiation. In contrast, this study addressed how high‐energy particle radiation (200‐MeV protons, simulating the effect of galactic cosmic rays and solar wind at depths of <4–5 cm) inﬂuences organic macromolecules in sediments. Speciﬁcally, we report the generation of organic‐acid radiolysis products after exposure to radiation doses equivalent to geological time scales (1–7 Myr). We found that formate and oxalate were produced from a variety of organic starting materials and mineral matrices. Unlike ultraviolet‐driven reactions that can invoke Fenton chemistry to produce organic acids, our work suggests that irradiation of semiconductor surfaces, such as TiO2 or possible clay minerals found on Mars, forms oxygen and hydroxyl radical species, which can break down macromolecules into organic acids. We also investigated the metastability of benzoate in multiple mineral matrices. Benzoate was added to samples prior to irradiation and persisted up to 500 kGys of exposure. Our ﬁndings suggest that organic acids are likely a major component of organic material buried at depth on Mars.

Fox, A. C.↗

NASA NTRS1978

Interconversion of biologically important carboxylic acids by radiation

The interconversion of a group of biologically important polycarboxylic acids (acetic, fumaric, malic, malonic, succinic, citric, isocitric, tricarballylic) under gamma-ray or ultraviolet radiation was investigated. The formation of high molecular weight compounds was observed in all cases. Succinic acid was formed in almost all radiolysis experiments. Citric, malonic, and succinic acids appeared to be relatively insensitive to radiation. Interconversion of the polycarboxylic acids studied may have occurred under the effect of radiation in the prebiotic earth.

Negron-Mendoza, A.↗

NASA NTRS1983

Pulse radiolysis of epoxy-based matrix materials

Electron beam pulse radiolysis (600 KeV, 3 nsec) experiments have been carried out on epoxy-based matrix materials. Time and wavelength resolved emission and transient absorption techniques as well as ESR studies have been utilized to identify and monitor short lived reactive intermediates resulting from energetic electron impact. An energy deactivation model based on the results of this work has been developed. Recombination of primary charged species is found to be fast, resulting in the formation of longer lived excited electronic states and radicals which control the subsequent energy deactivation.

Coulter, D. R.↗

NASA NTRS2014

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↗

NASA NTRS1988

Laboratory studies of irradiated nitrogen-methane mixtures - Applications to Triton

The characteristics of the near-IR spectrum of Triton is addressed in view of 0.8-2.5 micron laboratory transmission spectra obtained for methane dissolved in liquid nitrogen. It is found that, for methane concentrations greater than 3 percent of the saturation value, the collision-induced, 2.152-micron first-overtone band of molecular nitrogen is overshadowed by the methane band centered at 2.3 microns. While gamma-radiolysis of nitrogen-methane mixtures generates an unstable precipitate whose yellowish color is qualitatively similar to the yellow color of Triton, no specific absorption band in the precipitate can be unambiguously identified on Triton.

Piscitelli, J. R.↗

NASA NTRS2004

Radiolytic Model for Chemical Composition of Europa's Atmosphere and Surface

The overall objective of the present effort is to produce models for major and selected minor components of Europa s neutral atmosphere in 1-D versus altitude and in 2-D versus altitude and longitude or latitude. A 3-D model versus all three coordinates (alt, long, lat) will be studied but development on this is at present limited by computing facilities available to the investigation team. In this first year we have focused on 1-D modeling with Co-I Valery Shematovich s Direct Simulation Monte Carlo (DSMC) code for water group species (H2O, O2, O, OH) and on 2-D with Co-I Mau Wong's version of a similar code for O2, O, CO, CO2, and Na. Surface source rates of H2O and O2 from sputtering and radiolysis are used in the 1-D model, while observations for CO2 at the Europa surface and Na detected in a neutral cloud ejected from Europa are used, along with the O2 sputtering rate, to constrain source rates in the 2-D version. With these separate approaches we are investigating a range of processes important to eventual implementation of a comprehensive 3-D atmospheric model which could be used to understand present observations and develop science requirements for future observations, e.g. from Earth and in Europa orbit. Within the second year we expect to merge the full water group calculations into the 2-D version of the DSMC code which can then be extended to 3-D, pending availability of computing resources. Another important goal in the second year would be the inclusion of sulk and its more volatile oxides (SO, SO2).

Cooper, John F.↗

NASA NTRS1983

The reaction NH2 + PH3 yields NH3 + PH2 - Absolute rate constant measurement and implication for NH3 and PH3 photochemistry in the atmosphere of Jupiter

The rate constant is measured over the temperature interval 218-456 K using the technique of flash photolysis-laser-induced fluorescence. NH2 radicals are produced by the flash photolysis of ammonia highly diluted in argon, and the decay of fluorescent NH2 photons is measured by multiscaling techniques. For each of the five temperatures employed in the study, the results are shown to be indepenent of variations in PH3 concentration, total pressure (argon), and flash intensity. It is found that the rate constant results are best represented for T between 218 and 456 K by the expression k = (1.52 + or - 0.16) x 10 to the -12th exp(-928 + or - 56/T) cu cm per molecule per sec; the error quoted is 1 standard deviation. This is the first determination of the rate constant for the reaction NH2 + PH3. The data are compared with an estimate made in order to explain results of the radiolysis of NH3-PH3 mixtures. The Arrhenius parameters determined here for NH2 + PH3 are then contrasted with those for the corresponding reactions of H and OH with PH3.

Bosco, S. R.↗

NASA NTRS1983

The reaction NH2 + PH3 yields NH3 + PH2: Absolute rate constant measurement and implication for NH3 and PH3 photochemistry in the atmosphere of Jupiter

The rate constant is measured over the temperature interval 218-456 K using the technique of flash photolysis-laser-induced fluorescence. NH2 radicals are produced by the flash photolysis of ammonia highly diluted in argon, and the decay of fluorescent NH2 photons is measured by multiscaling techniques. For each of the five temperatures employed in the study, the results are shown to be independent of variations in PH3 concentration, total pressure (argon), and flash intensity. It is found that the rate constant results are best represented for T between 218 and 456 K by the expression k = (1.52 + or - 0.16) x 10 to the -12th exp(-928 + or - 56/T) cu cm per molecule per sec; the error quoted is 1 standard deviation. This is the first determination of the rate constant for the reaction NH2 + PH3. The data are compared with an estimate made in order to explain results of the radiolysis of NH3-PH3 mixtures. The Arrhenius parameters determined here for NH2 + PH3 are then constrasted with those for the corresponding reactions of H and OH with PH3.

Bosco, S. R.↗

NASA NTRS2011

New Modeling Approaches to Investigate Cell Signaling in Radiation Response

Ionizing radiation damages individual cells and tissues leading to harmful biological effects. Among many radiation-induced lesions, DNA double-strand breaks (DSB) are considered the key precursors of most early and late effects [1] leading to direct mutation or aberrant signal transduction processes. In response to damage, a flow of information is communicated to cells not directly hit by the radiation through signal transduction pathways [2]. Non-targeted effects (NTE), which includes bystander effects and genomic instability in the progeny of irradiated cells and tissues, may be particularly important for space radiation risk assessment [1], because astronauts are exposed to a low fluence of heavy ions and only a small fraction of cells are traversed by an ion. NTE may also have important consequences clinical radiotherapy [3]. In the recent years, new simulation tools and modeling approaches have become available to study the tissue response to radiation. The simulation of signal transduction pathways require many elements such as detailed track structure calculations, a tissue or cell culture model, knowledge of biochemical pathways and Brownian Dynamics (BD) propagators of the signaling molecules in their micro-environment. Recently, the Monte-Carlo simulation code of radiation track structure RITRACKS was used for micro and nano-dosimetry calculations [4]. RITRACKS will be used to calculate the fraction of cells traversed by an ion and delta-rays and the energy deposited in cells in a tissue model. RITRACKS also simulates the formation of chemical species by the radiolysis of water [5], notably the .OH radical. This molecule is implicated in DNA damage and in the activation of the transforming growth factor beta (TGF), a signaling molecule involved in NTE. BD algorithms for a particle near a membrane comprising receptors were also developed and will be used to simulate trajectories of signaling molecules in the micro-environment and characterize autocrine and paracrine cell communication and signal transduction.

Plante, Ianik↗