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NASA NTRS2019

Titan's Ionospheric Chemistry, Fullerenes, Oxygen, Galactic Cosmic Rays and the Formation of Exobiological Molecules on and within its Surfaces and Lakes

We discuss the formation of aerosols within Titan's thermosphere-ionosphere and the different chemical pathways. Negative ion measurements by the Cassini Plasma Spectrometer (CAPS) Electron Spectrometer (ELS) give evidence for formation of unsaturated anion carbon chains, while positive ion measurements of the Cassini Ion Neutral Mass Spectrometer (INMS) indicate formation of more aromatic cation hydrocarbons. There is presently no direct observational evidence for large neutral molecule growth in Titan's thermosphere-ionosphere. The hydrocarbon cations are expected to form Polycyclic Aromatic Hydrocarbons (PAH), those with the addition of nitrogen being called PAHNs. We theorize anion carbon chains can eventually become long enough to fold into fullerene C(60,70) carbon shells, of various charge states. Based on laboratory data the fullerenes can trap incoming O(sup +) magnetospheric ions that have relatively high energy collisions with the fullerenes and, once trapped, protect the oxygen atom from Titan's reducing thermosphere-ionosphere. The fullerenes can form into larger onion fullerenes and condense into larger embryo aerosols (i.e., m/q > 10,000 amu/q anions as observed by CAPS/ELS) eventually falling onto Titan's surface and precipitating to the bottom of its hydrocarbon lakes. Molecule production composed of H, C, N is known to occur in Titan's atmosphere with energy input from the magnetosphere, solar UV, and deeppenetrating irradiation from galactic cosmic rays (GCR). Space radiation effects by GCR irradiation of Titan's surface and lakes can lead to the manufacture of exobiological molecules with oxygen as the new ingredient. We have developed a model of galactic cosmic ray irradiation of Titan's atmosphere, surface, subsurface and bottoms of Titan lakes. GCR would provide further energy for processing of the aerosols into more complex organic forms such as tholins and precursor molecules for amino acids. A second process called hydrolysis then converts the precursor molecules into amino acids. Hydrolysis is provided via meteor impacts with size > 10 km and cryovolcanism both which can produce liquid water on Titan's surface for episodic periods > several 100 to 1000 years. Our model shows that GCR secondary particles can penetrate ~ 100 m below the ice surface (including the bottom of Titan's less dense hydrocarbon lakes ~ 150 m depths) and produce chemically significant dosages over very long timescales ~ 450 Myrs. The GCR model is combined with laboratory data from experiments in which dry methyl ices were irradiated to doses producing prebiotic amino acids such as glycine. The model calculations show glycine can form to ~ 2.5 ppb levels near the surface after ~450 Myrs of GCR proton irradiation and potentially to 5 ppb if heavy-ion GCRs up through Fe are included. If such molecules were detected, this would not only confirm this model but indicate that life forms different from ours may not be required.

Edward C. Sittler Jr↗
NASA NTRS2014

Carbon-Temperature-Water Change Analysis for Peanut Production Under Climate Change: A Prototype for the AgMIP Coordinated Climate-Crop Modeling Project (C3MP)

Climate change is projected to push the limits of cropping systems and has the potential to disrupt the agricultural sector from local to global scales. This article introduces the Coordinated Climate-Crop Modeling Project (C3MP), an initiative of the Agricultural Model Intercomparison and Improvement Project (AgMIP) to engage a global network of crop modelers to explore the impacts of climate change via an investigation of crop responses to changes in carbon dioxide concentration ([CO2]), temperature, and water. As a demonstration of the C3MP protocols and enabled analyses, we apply the Decision Support System for Agrotechnology Transfer (DSSAT) CROPGRO-Peanut crop model for Henry County, Alabama, to evaluate responses to the range of plausible [CO2], temperature changes, and precipitation changes projected by climate models out to the end of the 21st century. These sensitivity tests are used to derive crop model emulators that estimate changes in mean yield and the coefficient of variation for seasonal yields across a broad range of climate conditions, reproducing mean yields from sensitivity test simulations with deviations of ca. 2% for rain-fed conditions. We apply these statistical emulators to investigate how peanuts respond to projections from various global climate models, time periods, and emissions scenarios, finding a robust projection of modest (<10%) median yield losses in the middle of the 21st century accelerating to more severe (>20%) losses and larger uncertainty at the end of the century under the more severe representative concentration pathway (RCP8.5). This projection is not substantially altered by the selection of the AgMERRA global gridded climate dataset rather than the local historical observations, differences between the Third and Fifth Coupled Model Intercomparison Project (CMIP3 and CMIP5), or the use of the delta method of climate impacts analysis rather than the C3MP impacts response surface and emulator approach.

climate change↗
NASA NTRS2015

Basin-Scale Assessment of the Land Surface Energy Budget in the National Centers for Environmental Prediction Operational and Research NLDAS-2 Systems

This paper compares the annual and monthly components of the simulated energy budget from the North American Land Data Assimilation System phase 2 (NLDAS-2) with reference products over the domains of the 12 River Forecast Centers (RFCs) of the continental United States (CONUS). The simulations are calculated from both operational and research versions of NLDAS-2. The reference radiation components are obtained from the National Aeronautics and Space Administration Surface Radiation Budget product. The reference sensible and latent heat fluxes are obtained from a multitree ensemble method applied to gridded FLUXNET data from the Max Planck Institute, Germany. As these references are obtained from different data sources, they cannot fully close the energy budget, although the range of closure error is less than 15%formean annual results. The analysis here demonstrates the usefulness of basin-scale surface energy budget analysis for evaluating model skill and deficiencies. The operational (i.e., Noah, Mosaic, and VIC) and research (i.e., Noah-I and VIC4.0.5) NLDAS-2 land surface models exhibit similarities and differences in depicting basin-averaged energy components. For example, the energy components of the five models have similar seasonal cycles, but with different magnitudes. Generally, Noah and VIC overestimate (underestimate) sensible (latent) heat flux over several RFCs of the eastern CONUS. In contrast, Mosaic underestimates (overestimates) sensible (latent) heat flux over almost all 12 RFCs. The research Noah-I and VIC4.0.5 versions show moderate-to-large improvements (basin and model dependent) relative to their operational versions, which indicates likely pathways for future improvements in the operational NLDAS-2 system.

Energy↗
NASA NTRS2010

Synergism of Saturn, Enceladus and Titan and Formation of HCNO Exobiological Molecules

Saturn as a system has two very exotic moons Titan and Enceladus. Titan with energy input from Saturn's magnetosphere, solar UV irradiation, and cosmic rays can make HCN based molecules as discussed in earlier paper by [1]. Space radiation effects at both moons, and as coupled by the Saturn magnetosphere could cause an unexpected series of events leading to the evolution of biological models at Titan composed of HCNO with oxygen as the new ingredient. The "Old Faithful" model by [2] suggests that Enceladus, highly irradiated by Saturn magnetospheric electrons, has episodic ejections of water vapor driven by radiolytic oxidation gas products into Saturn's magnetosphere. At Titan Cassini discovered 1) that keV oxygen ions, evidently from Enceladus, are bombarding Titan's upper atmosphere [3] and 2) the discovery of heavy positive and negative ions within Titan's upper atmosphere [4]. Initial models of heavy ion formation in Titan's upper atmosphere invoked polymerization of aromatics such as Benzenes and their radicals to make PAHs [5], while a more recent model by [6] has raised the possibility of carbon chains forming from the polymerization of acetylene and its radicals to eventually make fullerenes. Laboratory measurements indicate that fullerenes, which are hollow carbon shells, can trap the keV oxygen and with the clustering of fullerenes and possible mixture with PAHs, some with nitrogen molecules, can make the larger aerosols with oxygen within them. Then with further ionizing irradiation from cosmic rays deep in the atmosphere "tholin" molecules are produced with all the molecular components present from which organic molecules can form. Among the molecular components are amino acids, the fundamental building blocks of life as we know it. This process maybe a common chemical pathway, both at the system level and at the molecular level, to form prebiotic and perhaps even biotic molecules. Such processes can be occurring throughout our universe, such as molecular clouds in the ISM.

Sittler, Edward C., Jr.↗
NASA NTRS2019

Evaluating Effects of Altered Gravity on the Nervous System Using D. melanogaster

A comprehensive understanding of the effects of spaceflight and altered gravity on human physiology is necessary for continued human space exploration and long-term space habitation. The oxidative stress response has been identified in astronauts exposed to short- and long-term space missions that are exposed to the multitude of stress factors of spaceflight, including altered gravity and radiation exposure. Reactive oxygen species (ROS) are byproducts of homeostatic cellular metabolism, yet when overproduced the oxidative stress response ensues, rendering molecules destructive causing cell death and inflammation. Controlling aberrant ROS production is necessary to prevent pathological consequences, in particular within the nervous system, since neurons are extremely sensitive overexpressed ROS insults. We hypothesize that exposure to altered gravity triggers the oxidative stress response, leading to impairments in the nervous system. In this study, we used a well-established spaceflight model organism, Drosophila melanogaster, to assess altered gravity associated changes in the nervous system using a ground-based hypergravity model. Acute hypergravity resulted in an induction of oxidative stress-related genes with an increase in reactive oxygen species (ROS) in fly brains (p<0.001). Also, qPCR analysis shows that parkin gene expression is significantly reduced in these fly brains(p<0.05). Additionally, chronic hypergravity resulted in depressed locomotor phenotype in these flies (p<0.05) in conjunction to decreased dopaminergic neuron counts (p<0.0001) and increased apoptosis in these fly brains (p<0.0001). Further, assessment of neurological changes, including the neuronal architecture, synaptic integrity and genetic regulation caused by hypergravity conditions were noted. Overall, our results validate chronic hypergravity simulation as a behavioral model to study spaceflight effects, and oxidative stress pathway as a potential avenue for countermeasure development for astronauts undergoing short- and long-term missions and for neurodegenerative research on Earth.

Mhatre, Siddhita↗
NASA NTRS2004

DNA in a Tunnel: A Comfy Spot for Recognition - or -The Structure of BsoBI Complexed with DNA. What can we Learn about Function via Structure Determination and how can this be Applied to Bone or Muscle Biology?

The structure and function of a biologically active molecule are related. To understand its function, it is necessary (but not always sufficient) to know the structure of the molecule. There are many ways of relating the molecular function with the structure. Mutation analysis can identify pertinent amino acids of an enzyme, or alternatively structure comparison of the of two similar molecules with different function may lead to understanding which parts are responsible for a functional aspect, or a series of "structural cartoons" - enzyme structure, enzyme plus substrate, enzyme with transition state analog, and enzyme with product - may give insight in the function of a molecule. As an example we will discuss the structure and function of the restriction enzyme BsoBI from Bacillus stearothemzophilus in complex with its cognate DNA. The enzyme forms a unique complex with DNA in that it completely encircles the DNA. The structure reveals the enzyme-DNA contacts, how the DNA is distorted compared with the canonical forms, and elegantly shows how two distinct DNA sequences can be recognized with the same efficiency. Based on the structure we may also propose a hypothesis how the enzymatic mechanism works. The knowledge gained thru studies such as this one can be used to alter the function by changing the molecular structure. Usually this is done by design of inhibitors specifically active against and fitting into an active site of the enzyme of choice. In the case of BsoBI one of the objectives of the study was to alter the enzyme specificity. In bone biology there are many candidates available for molecular study in order to explain, alter, or (temporarily) suspend activity. For example, the understanding of a pathway that negatively regulates bone formation may be a good target for drug design to stimulate bone formation and have good potential as the basis for new countermeasures against bone loss. In principle the same approach may aid muscle atrophy, radiation damage, immune response changes and other risks identified for long-duration Space travel.

vanderWoerd, Mark↗
NASA NTRS2018

Coordinating AgMIP Data and Models Across Global and Regional Scales for 1.5°C and 2.0°C Assessments

The Agricultural Model Intercomparison and Improvement Project (AgMIP) has developed novel methods for Coordinated Global and Regional Assessments (CGRA) of agriculture and food security in a changing world. The present study aims to perform a proof of concept of the CGRA to demonstrate advantages and challenges of the proposed framework. This effort responds to the request by the UN Framework Convention on Climate Change (UNFCCC) for the implications of limiting global temperature increases to 1.5°C and 2.0°C above pre-industrial conditions. The protocols for the 1.5°C/2.0°C assessment establish explicit and testable linkages across disciplines and scales, connecting outputs and inputs from the Shared Socio-economic Pathways (SSPs), Representative Agricultural Pathways (RAPs), Half a degree Additional warming, Prognosis and Projected Impacts (HAPPI) and Coupled Model Intercomparison Project Phase 5 (CMIP5) ensemble scenarios, global gridded crop models, global agricultural economics models, site-based crop models and within-country regional economics models. The CGRA consistently links disciplines, models and scales in order to track the complex chain of climate impacts and identify key vulnerabilities, feedbacks and uncertainties in managing future risk. CGRA proof-of-concept results show that, at the global scale, there are mixed areas of positive and negative simulated wheat and maize yield changes, with declines in some bread basket regions, at both 1.5°C and 2.0°C. Declines are especially evident in simulations that do not take into account direct CO2 effects on crops. These projected global yield changes mostly resulted in increases in prices and areas of wheat and maize in two global economics models. Regional simulations for 1.5°C and 2.0°C using site-based crop models had mixed results depending on the region and the crop. In conjunction with price changes from the global economics models, productivity declines in the Punjab, Pakistan, resulted in an increase in vulnerable households and the poverty rate. This article is part of the theme issue ‘The Paris Agreement: understanding the physical and social challenges for a warming world of 1.5°C above pre-industrial levels’.

interdisciplinary↗
NASA NTRS1993

Cellular responses to low-gravity: Pilot studies on suborbital rockets and orbiting spacecraft

The allocated funding supported, in part, experiments conducted on two Consort sounding rockets and five Shuttle flights. The primary parameters investigated were signal transduction in response to various mediators, cellular differentiation and metabolism in microgravity, and effect of microgravity on cytoskeletal morphology. Achievements include: demonstration of effect of spaceflight on the actin cytoskeleton in mouse osteoblasts and frog cells; confirmation that the T cell receptor-mediated signal transduction pathway in T lymphocytes is not affected by low-gravity compared to non-TCR-mediated stimulation (Con-A) which classically does not promote proliferative response; indication that microgravity may allow separation of proliferative signaling and secretory function in lymphocytes; demonstration that T lymphocytes and bone cells utilized less glucose indicating a shift in metabolism and confirming Spacelab results with WI-38 cells which used significantly less glucose, during spaceflight; confirmation that activation of human splenic B cells with a number of different mediators is not affected during spaceflight; demonstration of increased prostaglandin synthesis during reduced bone cell growth suggesting an effect of microgravity on prostaglandin-induced mitogenesis. The funding contributed significantly to the database described above and resulted in submission of six collaborative abstracts in 1993 (five to the ASGSB Annual Meeting and one to the ASCB Annual Meeting). Two abstracts were presented at the 1992 ASGSB Annual Meeting in Tucson. In addition, several peer reviewed papers are being generated and data will be included as background in preparation of future proposals, which hopefully will allow us to continue this type of extremely productive collaborative research.

Lewis, Marian L.↗
NASA NTRS2014

De Novo Synthesis and Functional Study of Primitive Polypeptides in the Prebiotic Protein World

DNA, RNA and proteins within a lipid-bound membrane are the core components of life, but the order of their appearance during the origin of life is still under debate. The widely accepted RNA World hypothesis states that RNA likely emerged prior to proteins and DNA since RNA can serve both replicative and catalytic roles. While biochemists have reproduced the synthesis, polymerization, and replication of nucleotides and RNA under controlled prebiotic conditions, it is clear that such complex organic molecules were are not present in significant amounts in the the starting prebiotic material on Earth either from endogenous production or meteoritic input. In contrast, amino acids are naturally abundant in various prebiotic contexts such as carbonaceous chondrites and Urey-Miller type experiments, and many studies have demonstrated that under plausible prebiotic conditions amino acids could condense or polymerize to give rise to short peptides. These findings support the basis of a Protein World hypothesis for life, however little has been done to study the functions of such primitive peptides. Here we present our novel synthetic biology-based approach to the de novo synthesis of billions of primitive peptidesproteins derived from a limited set of naturally abundant proteinogenic amino acids such as glycine, alanine, aspartic acid, glutamic acid, valine and serine. Of these peptides, the ones with divalent metal-binding capability are of particular interest and will be screened and identified. Certain divalent metals were likely present in prebiotic environments. Not only do they coordinate well with amino acids, but they also catalyze reactions, which are difficult to achieve in organic chemistry. Since D-chiral and non-proteinogenic amino acids are also abundant in the universe and may provide insight into the pathway by which life developed, we will also discuss methods to analyze primitive peptides consisting of these amino acids and D-chiral and non-proteinogenic amino acids. By understanding this naturalistic pathway, we will be able to better understand how life developed here on Earth. Since these amino acids are abundant in universe, this work provide insight into pathways by which life developed on Earth and, by extension, the probability of life arising elsewhere.

Fujishima, Kosuke↗
NASA NTRS2020

Titan's Ionospheric Chemistry, Fullerenes, Oxygen, Galactic Cosmic Rays and the Formation of Exobiological Molecules on and Within Its Surfaces and Lakes

We discuss the formation of aerosols within Titan's thermosphere-ionosphere and the different chemical pathways. Negative ion measurements by the Cassini Plasma Spectrometer (CAPS) Electron Spectrometer (ELS) give evidence for formation of unsaturated anion carbon chains, while positive ion measurements of the Cassini Ion Neutral Mass Spectrometer (INMS) indicate formation of more aromatic cation hydrocarbons. There is presently no direct observational evidence for large neutral molecule growth in Titan's thermosphere-ionosphere. The hydrocarbon cations are expected to form Polycyclic Aromatic Hydrocarbons (PAHs), those with the addition of nitrogen being called PAHNs. We theorize anion carbon chains can eventually become long enough to fold into fullerene C60,70 carbon shells, of various charge states. Based on laboratory data the fullerenes can trap incoming O+ magnetospheric ions that have relatively high energy collisions with the fullerenes and, once trapped, protect the oxygen atom from Titan's reducing thermosphere-ionosphere. The fullerenes can form into larger onion fullerenes and condense into larger embryo aerosols (i.e., m/q (mass-to-charge ratio) greater than 10,000 amu/q (atomic mass unit-to-charge ratio) anions as observed by CAPS/ELS) eventually falling onto Titan's surface and precipitating to the bottom of its hydrocarbon lakes. Molecule production composed of H, C, N is known to occur in Titan's atmosphere with energy input from the magnetosphere, solar UV (ultraviolet), and deep-penetrating irradiation from galactic cosmic rays (GCR). Space radiation effects by GCR irradiation of Titan's surface and lakes can lead to the manufacture of exobiological molecules with oxygen as the new ingredient. We have developed a model of galactic cosmic ray irradiation of Titan's atmosphere, surface, subsurface and bottoms of Titan lakes. GCR would provide further energy for processing of the aerosols into more complex organic forms such as tholins and precursor molecules for amino acids. A second process called hydrolysis then converts the precursor molecules into amino acids. Hydrolysis is provided via meteor impacts with size greater than 10 kilometers and cryovolcanism both which can produce liquid water on Titan's surface for episodic periods more than several 100 to 1000 years. Our model shows that GCR secondary particles can penetrate ~100 meters below the ice surface (including the bottom of Titan's less dense hydrocarbon lakes ~150-meter depths) and produce chemically significant dosages over very long timescales ~450 million years. The GCR model is combined with laboratory data from experiments in which dry methyl ices were irradiated to doses producing prebiotic amino acids such as glycine. The model calculations show glycine can form to ~2.5 parts-per-billion levels near the surface after ~450 million years of GCR proton irradiation and potentially to 5 parts-per-billion if heavy-ion GCRs up through Fe are included. If such molecules were detected, this would not only confirm this model but indicate that life forms different from ours may not be required.

Edward C. Sittler Jr↗
NASA NTRS2003

NOS II inhibition attenuates post-suspension hypotension in Sprague-Dawley rats

The reduction in mean arterial pressure observed in astronauts may be related to the impairment of autonomic function and/or excessive production of endothelium-derived relaxing factors. Here, we examined the role of a nitric oxide synthase II (NOS II) inhibitor AMT (2-amino-dihydro-6-methyl-4H-1,3-thiazine) against the post-suspension reduction in mean arterial pressure (MAP) in conscious male Sprague-Dawley rats. Direct MAP and heart rate were determined prior to tail-suspension, daily during the 7-day suspension and every 2 hrs post-suspension. Prior to release from suspension and at 2 and 4 hrs post-suspension, AMT (0.1 mg/kg), or saline, were administered intravenously. During the 7-day suspension, MAP was not altered, nor were there significant changes in heart rate. The reduction in MAP post-suspension in saline-treated rats was associated with significant increases in plasma nitric oxide and prostacyclin. 2-Amino-dihydro-6-methyl4H-1,3-thiazine reduced plasma nitric oxide levels, but not those of prostacyclin, attenuated the observed post-suspension reduction in MAP and modified the baroreflex sensitivity for heart rate. Thus, the post suspension reduction in mean arterial pressure is due, in part, to overproduction of nitric oxide, via the NOS II pathway, and alteration in baroreflex activity.

NASA Discipline Cardiopulmonary↗
NASA NTRS2011

Incorporating JULES into NASA's Land Information System (LIS) and Investigations of Land-Atmosphere Coupling

NASA's Land Information System (LIS; lis.gsfc.nasa.gov) is a flexible land surface modeling and data assimilation framework developed over the past decade with the goal of integrating satellite- and ground-based observational data products and advanced land surface modeling techniques to produce optimal fields of land surface states and fluxes. LIS features a high performance and flexible design, and operates on an ensemble of land surface models for extension over user-specified regional or global domains. The extensible interfaces of LIS allow the incorporation of new domains, land surface models (LSMs), land surface parameters, meteorological inputs, data assimilation and optimization algorithms. In addition, LIS has also been demonstrated for parameter estimation and uncertainty estimation, and has been coupled to the Weather Research and Forecasting (WRF) mesoscale model. A visiting fellowship is currently underway to implement JULES into LIS and to undertake some fundamental science on the feedbacks between the land surface and the atmosphere. An overview of the LIS system, features, and sample results will be presented in an effort to engage the community in the potential advantages of LIS-JULES for a range of applications. Ongoing efforts to develop a framework for diagnosing land-atmosphere coupling will also be presented using the suite of LSM and PBL schemes available in LIS and WRF along with observations from the U. S .. Southern Great Plains. This methodology provides a potential pathway to study factors controlling local land-atmosphere coupling (LoCo) using the LIS-WRF system, which will serve as a testbed for future experiments to evaluate coupling diagnostics within the community.

Santanello, Joseph↗
NASA NTRS2013

The Search for Nitrates on Mars by the Sample Analysis at Mars (SAM) Instrument

Planetary models suggest that nitrogen was abundant in the early Martian atmosphere as N2 but it was lost by sputtering and photochemical loss to space, impact erosion, and chemical oxidation to nitrates. A nitrogen cycle may exist on Mars where nitrates, produced early in Mars' history, may have been later decomposed back into N2 by the current impact flux. Nitrates are a fundamental source of nitrogen for terrestrial microorganisms, and they have evolved metabolic pathways to perform both oxidation and reduction to drive a complete biological nitrogen cycle. Therefore, the characterization of nitrogen in Martian soils is important to assess habitability of the Martian environment, particularly with respect to the presence of nitrates. The only previous mission that was designed to search for soil nitrates was the Phoenix mission but N-containing species were not detected by TEGA or the MECA WCL. Nitrates have been tentatively identified in Nakhla meteorites, and if nitrogen was oxidized on Mars, this has important implications for the habitability potential of Mars. Here we report the results from the Sample Analysis at Mars (SAM) instrument suite aboard the Curiosity rover during the first year of surface operations in Gale Crater. Samples from the Rocknest aeolian deposit and sedimentary rocks (John Klein) were heated to approx 835degC under helium flow and the evolved gases were analyzed by MS and GC-MS. Two and possibly three peaks may be associated with the release of m/z 30 at temperatures ranging from 180degC to 500degC. M/z 30 has been tentatively identified as NO; other plausible contributions include CH2O and an isotopologue of CO, 12C18O. NO, CH2O, and CO may be reaction products of reagents (MTBSTFA/DMF) carried from Earth for the wet chemical derivatization experiments with SAM and/or derived from indigenous soil nitrogenated organics. Laboratory analyses indicate that it is also possible that <550degC evolved NO is produced via reaction of HCl with nitrates arising from the decomposition of perchlorates. All sources of m/z 30 whether it be martian or terrestrial will be considered and their implications for Mars will be discussed.

Navarro-Gonzalez, Rafael↗
NASA NTRS2023

Natural sunlight-driven oxidation of Mn 2+ (aq) and heterogeneous formation of Mn oxides on hematite

The oxidation of dissolved Mn 2+ (aq) plays a critical role in driving manganese cycles and regulating the fate of essential elements and contaminants in environmental systems. Based on sluggish oxidation rate, abiotic processes have been considered less effective oxidation pathway for manganese oxidation in environmental systems. Interestingly, a recent study (Jung et al., 2021) has shown that the rapid photochemical oxidation of Mn 2+ (aq) could be a feasible scenario to uncover the potential significance of abiotic Mn 2+ (aq) oxidation. Nevertheless, the significance of photochemical oxidation of Mn 2+ (aq) under natural sunlight exposure remains unclear. Here, we demonstrate the rapid photocatalytic oxidation of Mn 2+ (aq) and the heterogeneous growth of tunnel-structured Mn oxides under simulated freshwater and seawater conditions in the presence of natural sunlight and hematite. The natural sunlight-driven photocatalytic oxidation of Mn 2+ (aq) by hematite showed kinetic constants of 1.02 h -−1 and 0.342 h −1 under freshwater and seawater conditions, respectively. The natural sunlight-driven photocatalytic oxidation rates are quite comparable to the results obtained from the previous laboratory test using artificial sunlight, which has ∼4.5 times stronger light intensity. It is likely because of ∼5.5 times larger light exposure area in the natural sunlight-driven photocatalytic oxidation than that of the laboratory test using artificial sunlight. We also elucidate the roles of cation species in controlling the oxidation rate of Mn 2+ (aq) and the crystalline structure of Mn oxide products. Specifically, in the presence of large amounts of cations, the oxidation rate of Mn 2+ (aq) was slower likely because of competitive adsorption. Furthermore, our findings highlight that Mn 2+ contributes significantly to the formation of large-tunneled Mn oxides. These results illuminate the importance of abiotic photocatalytic processes in controlling the redox chemistry of Mn in real environmental aqueous systems on the oxidation of Mn 2+ (aq), and provide an environmentally sustainable approach to effectively remediate water contaminated with Mn 2+ (aq) using natural sunlight.

Junyeong Choi↗
NASA NTRS2018

Compound-Specific Carbon Isotope Compositions of Aldehydes and Ketones in the Murchison Meteorite

Compound-specific carbon isotope analysis (delta(exp 13)C) of meteoritic organic compounds can be used to elucidate the abiotic chemical reactions involved in their synthesis. The soluble organic content of the Murchison carbonaceous chondrite has been extensively investigated over the years, with a focus on the origins of amino acids and the potential role of Strecker-cyanohydrin synthesis in the early solar system. Previous delta(exp 13)C investigations have targeted alpha-amino acid and alpha-hydroxy acid Strecker products and reactant HCN; however, delta(exp 13)C values for meteoritic aldehydes and ketones (Strecker precursors) have not yet been reported. As such, the distribution of aldehydes and ketones in the cosmos and their role in prebiotic reactions have not been fully investigated. Here, we have applied an optimized O-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine (PFBHA) derivatization procedure to the extraction, identification, and delta(exp 13)C analysis of carbonyl compounds in the Murchison meteorite. A suite of aldehydes and ketones, dominated by acetaldehyde, propionaldehyde, and acetone, were detected in the sample. delta(exp 13)C values, ranging from -10.0(0/00) to +66.4(0/00), were more (exp 13)C-depleted than would be expected for aldehydes and ketones derived from the interstellar medium, based on interstellar (exp 12)C/(exp 13)C ratios. These relatively (exp 13)C-depleted values suggest that chemical processes taking place in asteroid parent bodies (e.g., oxidation of the IOM) may provide a secondary source of aldehydes and ketones in the solar system. Comparisons between delta(exp 13)C compositions of meteoritic aldehydes and ketones and other organic compound classes were used to evaluate potential structural relationships and associated reactions, including Strecker synthesis and alteration-driven chemical pathways.

meteoritic organic compounds↗
NASA NTRS2014

Section 508 Electronic Information Accessibility Requirements for Software Development

Section 508 Subpart B 1194.21 outlines requirements for operating system and software development in order to create a product that is accessible to users with various disabilities. This portion of Section 508 contains a variety of standards to enable those using assistive technology and with visual, hearing, cognitive and motor difficulties to access all information provided in software. The focus on requirements was limited to the Microsoft Windows® operating system as it is the predominant operating system used at this center. Compliance with this portion of the requirements can be obtained by integrating the requirements into the software development cycle early and by remediating issues in legacy software if possible. There are certain circumstances with software that may arise necessitating an exemption from these requirements, such as design or engineering software using dynamically changing graphics or numbers to convey information. These exceptions can be discussed with the Section 508 Coordinator and another method of accommodation used.

Pathways↗
NASA NTRS2017

Pathways to Meteoritic Glycine and Methylamine

Glycine and methylamine are meteoritic water-soluble organic compounds that provide insights into the processes that occurred before, during, and after the formation of the Solar System. Both glycine and methylamine and many of their potential synthetic precursors have been studied in astrophysical environments via observations, laboratory experiments, and modeling. Despite these studies, the synthetic mechanisms for their formation leading to their occurrence in meteorites remain poorly understood. Typical 13C-isotopic values ((delta)13C) of meteoritic glycine and methylamine are 13C-enriched relative to their terrestrial counterparts; thus, analyses of their stable carbon isotopic compositions (13C/12C) may be used not only to assess terrestrial contamination in meteorites but also to provide information about their synthetic routes inside the parent body. Here, we examine potential synthetic routes of glycine and methylamine from a common set of precursors present in carbonaceous chondrite meteorites, using data from laboratory analyses of the well-studied CM2 Murchison meteorite. Several synthetic mechanisms for the origins of glycine and methylamine found in carbonaceous chondrites may be possible, and the prevalence of these mechanisms will largely depend on (a) the molecular abundance of the precursor molecules and (b) the levels of processing (aqueous and thermal) that occurred inside the parent body. In this work, we also aim to contextualize the current knowledge about gas-phase reactions and irradiated ice grain chemistry for the synthesis of these species through parent body processes. Our evaluation of various mechanisms for the origins of meteoritic glycine and methylamine from simple species shows what work is still needed to evaluate both the abundances and isotopic compositions of simpler precursor molecules from carbonaceous chondrites as well as the effects of parent body processes on those abundances and isotopic compositions. The analyses presented here combined with the indicated measurements will aid a better interpretation of quantitative analysis of reaction rates, molecular stability, and distribution of organic products from laboratory simulations of interstellar ices, astronomical observations, and theoretical modeling.

interstellar ice↗
NASA NTRS2003

Correction to "Asian chemical Outflow to the Pacific in Spring: Origins, Pathways, and Budgets" by Isabelle Bey et al.

We analyze the Asian outflow of CO, ozone, and nitrogen oxides (NOx) to the Pacific in spring by using the GEOS-CHEM global three-dimensional model of tropospheric chemistry and simulating the Pacific Exploratory Mission-West (PEM-West B) aircraft mission in February-March 1994. The GEOS-CHEM model uses assimilated meteorological fields from the NASA Goddard Earth Observing System (GEOS). It reproduces relatively well the main features of tropospheric ozone, CO, and reactive nitrogen species observed in PEM-West B, including latitudinal and vertical gradients of the Asian pollution outflow over the western Pacific although simulated concentrations of CO tend to be too low (possibly because biogenic sources are underestimated). We use CO as a long-lived tracer to diagnose the processes contributing to the outflow. The highest concentrations in the outflow are in the boundary layer (0-2 km), but the strongest outflow fluxes are in the lower free troposphere (2-5 km) and reflect episodic lifting of pollution over central and eastern China ahead of eastward moving cold fronts. This frontal lifting, followed by westerly transport in the lower free troposphere, is the principal process responsible for export of both anthropogenic and biomass burning pollution from Asia. Anthropogenic emissions from Europe and biomass burning emissions from Africa make also major contributions to the Asian outflow over the western Pacific; European sources dominate in the lower troposphere north of 40 degrees N, while African sources are important in the upper troposphere at low latitudes. For the period of PEM-West B (February-March) we estimate that fossil fuel combustion and biomass burning make comparable contributions to the budgets of CO, ozone, and NO, in the Asian outflow. We find that 13% of NO, emitted in Asia is exported as NO, or PAN, a smaller fraction than for the United States because of higher aerosol concentrations that promote heterogeneous conversion of NOx to HNO3. Production and export of ozone from Asia in spring is much greater than from the United States because of the higher photochemical activity.

Bey, Isabelle↗