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NASA NTRS1994

The meteoritic record of presolar and early solar system organic chemistry

Carbon, hydrogen, and nitrogen isotopic analyses of various classes of organic compounds done in collaboration with Epstein and Krishnamurthy (Caltech) have shown these compounds to be enriched to varying degrees in the heavier isotopes. These results, in particular the large deuterium enrichments, have been interpreted as indicating an interstellar origin for the meteorite compounds or their precursors. Such isotopic fractionations, of hydrogen especially, are characteristic of low temperature ion-molecule reactions in cold interstellar clouds. There is also evidence from the large corresponding suites of alpha-amino and alpha-hydroxy acids found in meteorites suggesting that aqueous phase chemistry on the meteorite parent body played an important role in the formation of these compounds. These data support the hypothesis that interstellar compounds survived in the solar nebula at a radial distance corresponding to the asteroid belt, were incorporated into the parent body in icy, volatile-rich, planetesinals, and underwent further reactions during a period of aqueous activity within the early parent body to give the present suite of meteorite compounds. This formation hypothesis will be discussed and the results of recent isotopic and molecular analyses bearing on it will be presented.

Cronin, John R.↗

NASA NTRS2003

Emissions of Trace Gases and Particles from Savanna Fires in Southern Africa

Airborne measurements made on initial smoke from 10 savanna fires in southern Africa provide quantitative data on emissions of 50 gaseous and particulate species, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, ammonia, dimethyl sulfide, nonmethane organic compounds, halocarbons, gaseous organic acids, aerosol ionic components, carbonaceous aerosols, and condensation nuclei (CN). Measurements of several of the gaseous species by gas chromatography and Fourier transform infrared spectroscopy are compared. Emission ratios and emission factors are given for eight species that have not been reported previously for biomass burning of savanna in southern Africa (namely, dimethyl sulfide, methyl nitrate, five hydrocarbons, and particles with diameters from 0.1 to 3 microns). The emission factor that we measured for ammonia is lower by a factor of 4, and the emission factors for formaldehyde, hydrogen cyanide, and CN are greater by factors of about 3, 20, and 3 - 15, respectively, than previously reported values. The new emission factors are used to estimate annual emissions of these species from savanna fires in Africa and worldwide.

Sinha, Parikhit↗

NASA NTRS2011

Meteorites, Organics and Fischer-Tropsch Type Reaction: Production and Destruction

There has been an ongoing debate about the relative importance about the various chemical reactions that fonned organics in the early solar system. One proposed method that has long been recognized as a potential source of organics is Fischer-Tropsch type (FTT) synthesis. This process is commonly used in industry to produce fuels (i.e., complex hydrocarbons) by catalytic hydrogenation of carbon monoxide. Hill and Nuth were the first to publish results of FTT experiments that also included Haber-Bosch (HB) processes (hydrogenation of nitrogen. Their findings included the production of nitrilebearing compounds as well as trace amounts of methyl amine. Previous experience with these reactions revealed that the organic coating deposited on the grains is also an efficient catalyst and that the coating is composed of insoluble organic matter (10M) and could be reminiscent of the organic matrix found in some meteorites. This current set of FTT-styled experiments tracks the evolution of a set of organics, amino acids, in detail.

Johnson, Natasha M.↗

NASA NTRS2014

Surface Ozone Variability and Trends over the South African Highveld from 1990 to 2007

Surface ozone is a secondary air pollutant formed from reactions between nitrogen oxides (NOx = NO + NO2) and volatile organic compounds in the presence of sunlight. In this work we examine effects of the climate pattern known as the El Niño-Southern Oscillation (ENSO) and NOx variability on surface ozone from 1990 to 2007 over the South African Highveld, a heavily populated region in South Africa with numerous industrial facilities. Over summer and autumn (December-May) on the Highveld, El Niño, as signified by positive sea surface temperature (SST) anomalies over the central Pacific Ocean, is typically associated with drier and warmer than normal conditions favoring ozone formation. Conversely, La Niña, or negative SST anomalies over the central Pacific Ocean, is typically associated with cloudier and above normal rainfall conditions, hindering ozone production. We use a generalized regression model to identify any linear dependence that the Highveld ozone, measured at five air quality monitoring stations, may have on ENSO and NOx. Our results indicate that four out of the five stations exhibit a statistically significant sensitivity to ENSO at some point over the December-May period where El Niño amplifies ozone formation and La Niña reduces ozone formation. Three out of the five stations reveal statistically significant sensitivity to NOx variability, primarily in winter and spring. Accounting for ENSO and NOx effects throughout the study period of 18 years, two stations exhibit statistically significant negative ozone trends in spring, one station displays a statistically significant positive trend in August, and two stations show no statistically significant change in surface ozone.

NOx↗

NASA NTRS2021

COVID-19 Crisis Reduces Free Tropospheric Ozone Across the Northern Hemisphere

Throughout spring and summer 2020, ozone stations in the northern extratropics recorded unusually low ozone in the free troposphere. From April to August, and from 1 to 8 kilometers altitude, ozone was on average 7% (≈4 nmol/mol) below the 2000–2020 climatological mean. Such low ozone, over several months, and at so many stations, has not been observed in any previous year since at least 2000. Atmospheric composition analyses from the Copernicus Atmosphere Monitoring Service and simulations from the NASA GMI model indicate that the large 2020 springtime ozone depletion in the Arctic stratosphere contributed less than one-quarter of the observed tropospheric anomaly. The observed anomaly is consistent with recent chemistry-climate model simulations, which assume emissions reductions similar to those caused by the COVID-19 crisis. COVID-19 related emissions reductions appear to be the major cause for the observed reduced free tropospheric ozone in 2020.

COVID-19↗

NASA NTRSDate not supplied

Quantifying the benefits of improved satellite remote-sensing observations for inverse modeling of NOx and NMVOC emissions

This study aims to demonstrate the benefits of using novel high spatiotemporal retrieval products from newer satellites for top-down emission estimates of nitrogen oxides (NO x ) and non-methane volatile organic compounds (NMVOCs) for the summer of 2019 over the contiguous United States. Recent satellite retrievals have not only advanced spatiotemporal resolution but also greatly reduced error and uncertainty due to reduced noise in the retrievals compared to spaceborne sensors launched in the past. We applied inverse modeling techniques using tropospheric nitrogen dioxide (NO 2 ) and formaldehyde (H-CHO) column retrieval products from the Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI) in conjunction with the Weather Research Forecast and Community Multiscale Air Quality Modeling system (WRF-CMAQ). In order to provide a better representation of background chemical composition and avoid misalignment of emission adjustment, we applied monthly scaling factors for ozone (O 3 ) and CO boundary concentrations in addition to the inclusion of lightning and aviation emissions. Satellite-constrained NO x and NMVOCs posterior emissions showed a mitigated discrepancy between observed and modeled columns. The improvement in the model performance was greater when using TROPOMI, primarily benefiting from reduced errors/biases of the satellite retrievals that enabled us to explore corresponding changes in O 3 concentrations and production sensitivity regimes using the ratio of H-CHO and NO 2 .

remote sensing↗

NASA NTRS2013

Tropospheric Ozone Changes, Radiative Forcing and Attribution to Emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (+/-1 standard deviation) in RFs of +/-17%. Three different radiation schemes were used - we find differences in RFs between schemes (for the same ozone fields) of +/-10 percent. Applying two different tropopause definitions gives differences in RFs of +/-3 percent. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of +/-30 percent for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44+/-12 percent), nitrogen oxides (31 +/- 9 percent), carbon monoxide (15 +/- 3 percent) and non-methane volatile organic compounds (9 +/- 2 percent); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m(−2) DU(−1), a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m(−2); relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

climate change↗

NASA NTRS1981

The validation of LIMS ozone profiles using correlative rocket, ECC, and Dobson data sets

The Limb Infrared Monitor of the Stratosphere (LIMS) experiment is a limb scanning infrared sounder designed to measure vertical temperature profiles and the concentrations of key chemical compounds which are important in the stratospheric ozone-nitrogen photochemistry. Preliminary ozone profiles are being intercompared with correlative rocket and balloonsonde ozone data sets as part of the Nimbus 7 LIMS data validation activity. The LIMS ozone retrievals extend from the lower mesosphere to the tropopause (or cloud-top altitudes). In this paper, preliminary statistics of comparisons of ECC (electrochemical concentration cell) ozonesonde and rocket ozone profiles with LIMS ozone profiles are presented. ECC ozonesonde data taken at times of LIMS overpasses are also used to extend the LIMS retrieval down to ground level. Each combined profile is then integrated to obtain total column ozone. These integrated results are compared to Dobson data obtained at approximately the same time and location.

Remsberg, E. E.↗

NASA NTRS2004

Space-Based Diagnosis of Surface Ozone Sensitivity to Anthropogenic Emissions

We present a novel capability in satellite remote sensing with implications for air pollution control strategy. We show that the ratio of formaldehyde columns to tropospheric nitrogen dioxide columns is an indicator of the relative sensitivity of surface ozone to emissions of nitrogen oxides (NO(x) = NO + NO2) and volatile organic compounds (VOCs). The diagnosis from these space-based observations is highly consistent with current understanding of surface ozone chemistry based on in situ observations. The satellite-derived ratios indicate that surface ozone is more sensitive to emissions of NO(x) than of VOCs throughout most continental regions of the Northern Hemisphere during summer. Exceptions include Los Angeles and industrial areas of Germany. A seasonal transition occurs in the fall when surface ozone becomes less sensitive to NOx and more sensitive to VOCs.

Martin, Randall V.↗

NASA NTRS2019

Mid-21st Century Ozone Air Quality and Health Burden in China Under Emissions Scenarios and Climate Change

Despite modest emissions reductions of air pollutants in recent years, China still suffers from poor air quality, and the outlook for future air quality in China is uncertain. We explore the impact of two disparate 2050 emissions scenarios relative to 2015 in the context of a changing climate with the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 (GFDL-AM3) chemistry-climate model. We impose the same near-term climate change for both emission scenarios by setting global sea surface temperature (SST) and sea ice cover (SIC) to the average over 2010–2019 and 2046–2055, respectively, from a three-member ensemble of GFDL coupled climate model simulations under the RCP8.5 (Representative Concentration Pathway) scenario. By the 2050s, annual mean surface ozone increases throughout China by up to 8 ppbv from climate change alone (estimated by holding air pollutants at 2015 levels while setting SIC and SST to 2050 conditions in the model) and by 8–12 ppbv in a scenario in which emissions of ozone precursors nitrogen oxides (NO (sub x) ) and anthropogenic volatile organic compounds (VOCs) increase by ~10%. In a scenario in which NO (sub x) and anthropogenic VOC emissions decline by 60%, annual mean surface ozone over China decreases by 16–20 ppbv in the 2050s relative to the 2010s. The ozone increase from climate change alone results in an additional 62 000 premature deaths in China as compared to 330 000 fewer premature deaths by the 2050s under a strong emissions mitigation scenario. In springtime over Southwestern China in the 2050s, the model projects 9–12 ppbv enhancements to surface ozone from the stratosphere (diagnosed with a model tracer) and from international anthropogenic emissions (diagnosed by differencing AM3 simulations with the same emissions within China but higher versus lower emissions in the rest of the world). Our findings highlight the effectiveness of emissions controls in reducing the health burden in China due to air pollution, and also the potential for climate change and rising global emissions to offset, at least partially, some of the ozone decreases attained with regional emission reductions in China.

Westervelt, D. M.↗

NASA NTRSDate not supplied

Changes in the Ozone Chemical Regime Over the Contiguous United States Inferred By the Inversion of NOx and VOC Emissions Using Satellite Observation

To investigate changes in the ozone (O3) chemical production regime over the contiguous United States (CONUS) with accurate knowledge of concentrations of its precursors, we applied an inverse modeling technique with Ozone Monitoring Instrument (OMI) tropospheric nitrogen dioxide (NO2) and total formaldehyde (HCHO) retrieval products in the summers of 2011, 2014, and 2017, years in which United States National Emission Inventory were based. The inclusion of dynamic chemical lateral boundary conditions and lightning-induced nitric oxide emissions significantly account for the contribution of background sources in the free troposphere. Satellite-constrained nitrogen oxide (NOx) and non-methane volatile organic compounds (NMVOCs) emissions mitigate the discrepancy between satellite and modeled columns: the inversion suggested 2.33-2.84 (1.07-1.34) times higher NOx over the CONUS (over urban regions) and 0.28-0.81 times fewer NMVOCs emissions over the southeastern United States. The model-derived HCHO/NO2 column ratio shows gradual spatial changes in the O3 production regime near urban cores relative to previously defined threshold values representing NOx and VOC sensitive conditions. We also found apparent shifts from the NOx-saturated regime to the transition regime (or the transition regime to the NOx-limited regime) over the major cities in the western United States. In contrast, rural areas, especially in the east-southeastern United States, exhibit a decreased HCHO/NO2 column ratio by -1.30 ± 1.71 with a reduction in HCHO column primarily driven by meteorology, becoming sensitive to VOC emissions. Results show that incorporating satellite observations into numerical modeling could help policymakers implement appropriate emission control policies for O3 pollution.

HCHO/NO2 factorInverse modelingOzone chemical regi↗

NASA NTRS1973

Chemical reactivity of hydrogen, nitrogen, and oxygen atoms at temperatures below 100 k

The synthesis of unusual compounds by techniques employing cryogenic cooling to retard their very extreme reactivity was investigated. Examples of such species that were studied are diimide (N2H2), cyclobutadiene (C4H4), cyclopropanone (C3H4O), oxirene (C2H2O), and many others. Special purpose cryogenically cooled inlet arrangements were designed such that the analyses incurred no warm-up of the cold, and frequently explosively unstable, compounds. Controlled energy electron impact techniques were used to measure critical potentials and to develop the molecular energetics and thermodynamics of these molecules and to gain some insight into their kinetic characteristics as well. Three and four carbon strained ring molecules were studied. Several reactions of oxygen and hydrogen atoms with simple molecules of H, N, C, and O in hard quench configurations were studied. And the quench stabilization of BH3 was explored as a model system in cryochemistry.

Mcgee, H. A., Jr.↗

NASA NTRS2026

Molecular Inventory and Comparative Organic Profiling of A Homogenized Aggregate Sample From Asteroid (101955) Bennu

Evaluating the distribution and diversity of solvent-soluble organic molecules in extraterrestrial materials provide information about the physicochemical environments where prebiotic chemistry occurred and is essential for assessing the inventory of prebiotic compounds available to the early Earth. In this work, we conducted a comprehensive molecular characterization of solvent-soluble organic compounds in a homogenized aggregate sample (ID: OREX-800107-128) of unsorted regolith from asteroid (101955) Bennu returned by NASA’s OSIRIS-REx mission. Using two-dimensional gas chromatography coupled with high-resolution time-of-flight mass spectrometry (GC×GC-HRMS), we identified 87 organic compounds across several molecular classes, including alkanes, polycyclic aromatic hydrocarbons, and nitrogen-, oxygen-, and sulfur-bearing species. Comparison with the organic inventory of CI (Orgueil), C2-ungrouped (Tagish Lake and Tarda), and CM2 (Murchison) carbonaceous chondrites revealed that Bennu sample OREX-800107-128 is most similar to Tagish Lake and Tarda yet compositionally distinct from all of these meteorites. This Bennu sample exhibits a relatively high abundance of low-molecular-weight aromatics (e.g., toluene), pyridine derivatives, and sulfur species such as dimethyl sulfite, consistent with episodic low-temperature aqueous alteration. The presence of these organic compounds suggests that this material experienced chemically diverse processes in the parent body conducive to complex organic synthesis, including aldol condensation reactions responsible for N- and O-bearing compounds. We also compared the molecular distributions of this Bennu sample and previously analyzed samples from (162173) Ryugu to assess potential common origins between these two carbonaceous asteroids. Bennu shows more chemically diverse and nitrogen-rich organic materials than Ryugu. While both asteroids share broadly similar primitive compositions, the observed chemical differences indicate distinct evolutionary histories within a likely common formation environment though whether Bennu and Ryugu derive from a single compositionally heterogeneous parent body or from multiple closely related progenitors remains unresolved. Further detailed comparative analyses of material from Bennu, Ryugu, and specific carbonaceous meteorites (e.g., Tagish Lake and Tarda) will provide new insights into how the N-rich molecular profile observed in Bennu samples was formed and evolved in the outer Solar System.

sample return↗

NASA NTRS1968

Could life originate now?

Abiogenesis, discussing hydrogen, oxygen, carbon, nitrogen and sulfur conversion into amino acids for simple organic compounds formation

Fox, S. W.↗

NASA NTRS1972

Review of jet engine emissions.

The various constituents in jet engine exhaust during typical takeoff or cruise conditions are presented in a table. The categories considered include inerts and unreacted oxygen from air, products of complete combustion of fuel, products of incomplete combustion, oxides of nitrogen formed during the heating of air, and elements or compounds derived from sulfur and trace metals present in kerosene fuel. Typical jet engine emission characteristics are discussed together with the effect of operating variables on emissions, and combustor design techniques to reduce emissions. Particular attention is given to emissions in the upper atmosphere, and to methods to reduce nitric oxide emissions.

Grobman, J. S.↗

NASA NTRS1987

Superconductivity at 93 K in a new mixed-phase Y-Ba-Cu-O compound system at ambient pressure

A stable and reproducible superconductivity transition between 80 and 93 K has been achieved and maintained in a Y-Ba-Cu-O compound system at ambient pressure in a simple liquid-nitrogen Dewar. An upper critical field Hc2(0) estimate of between 80 and 180 T is obtained, and the paramagnetic limiting field at 0 K for a sample with a T(c) of about 90 K is 165 T. It is suggested that the lattice parameters, the valence ratio, and the sample treatments all play a role in achieving superconductivity above 77 K.

Wu, M. K.↗

NASA NTRS1990

Carbon-rich particles in Comet Halley

The majority of particles detected in the coma of Comet Halley contain carbon atoms; many of these grains appear to consist preponderately or only of light elements. These light-element particles may be composed of organic compounds. Of the possible combinations of the elements hydrogen, carbon, nitrogen, and oxygen, numerous examples are found of particles containing the combinations (H,C,O,N), (H,C,N), (H,C,O), and (H,C). These results may bear on the recent detection of polyoxymethylene fragments, the observation of cyanojets (CN patterns consistent with release from solid particles), the possible presence of cyanopolyacetylenes or HCN polymer and the make-up of the CHON particles. If cometary matter could reach the surface of the earth without complete disruption, these diverse organic and mixed particles could create unique microenvironments, possibly with significant or even pivotal prebiotic chemical activity. Here a speculative insight into possible relationships between carbon in comets and carbon in life is given, as well as a brief overview of on-going analysis of data from the highly successful Particle Impact Analyzer (PIA) experiment flown on the Giotto spacecraft for the flyby of Comet Halley (development and implementation of PIA was under the direction of J. Kissel of the Max Planck Institute for Kernphysik, Heidelberg). PIA is a time-of-flight analyzer which obtains mass spectra of ions from individual particles impacting on a Pt-Ag foil target within the instrument.

Clark, Benton C.↗

NASA NTRS1991

Meissner-Effect Stepping Motor

Proposed stepping motor derives torque from diamagnetic repulsion produced by Meissner effect - exclusion of magnetic field from interior of superconductor. Design of motor takes advantage of silver-doped YB2Cu3O and other compounds superconductive at temperatures as high as that of liquid nitrogen. Skin of rotor cooled below its superconducting-transition temperature by liquid nitrogen. O-rings prevent leaks of liquid nitrogen from rotor. Weight, cost, and maintenance reduced.

Robertson, Glen A.↗