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NASA NTRS2013

Pre- and Post-perihelion Observations of C/2009 P1 (Garradd): Evidence for an Oxygen-rich Heritage?

We conducted pre- and post-perihelion observations of Comet C/2009 P1 (Garradd) on UT 2011 October 13 and 2012 January 8, at heliocentric distances of 1.83 and 1.57 AU, respectively, using the high-resolution infrared spectrometer (NIRSPEC) at the Keck II 10-m telescope on Mauna Kea, HI. Pre-perihelion, we obtained production rates for nine primary volatiles (native ices): H2O, CO, CH3OH, CH4, C2H6, HCN, C2H2, H2CO, and NH3. Post-perihelion, we obtained production rates for three of these (H2O, CH4, and HCN) and sensitive upper limits for three others (C2H2, H2CO, and NH3). CO was enriched and C2H2 was depleted, yet C2H6 and CH3OH were close to their currentmean values asmeasured in a dominant group of Oort cloud comets. This may indicate processing of its pre-cometary ices in a relatively oxygen-rich environment. Our measurements indicate consistent pre- and post-perihelion abundance ratios relative to H2O, suggesting we were measuring compositional homogeneity among measured species to the depths in the nucleus sampled. However, the overall gas production was lower post-perihelion despite its smaller heliocentric distance on January 8. This is qualitatively consistent with other studies of C/2009 P1, perhaps due to seasonal differences in the heating of one or more active regions on the nucleus. On October 13, the water profile showed a pronounced excess towards the Sun-facing hemisphere that was not seen in other molecules, including H2O on January 8, nor in the dust continuum. Inter-comparison of profiles from October 13 permitted us to quantify contributions due to release of H2O from the nucleus, and fromits release in the coma. This resulted in the latter source contributing 25-30% of the total observed water within our slit, which covered roughly +/-300 km by +/-4500 km from the nucleus. We attribute this excess H2O, which peaked at a mean projected distance of 1300-1500 km from the nucleus, to release from water-rich, relatively pure icy grains

Volatile composition↗

NASA NTRS2014

Changes in Global Tropospheric OH Expected as a Result of Climate Change Over the Last Several Decades

The oxidizing capacity of the troposphere is controlled primarily by the abundance of hydroxyl radical (OH). The global mean concentration of OH, [OH]_GLOBAL, inferred from measurements of methyl chloroform, has remained relatively constant during the past several decades, despite rising levels of CH4 that should have led to a steady decline. Here we examine other factors that may have affected [OH]_GLOBAL, such as the changing overhead burden of stratospheric O3 using observations from OMI, TOMS and SBUV; rising tropospheric H2O using observations from AIRS and reanalysis fields from MERRA; and widening of the climatological tropics using widening rate estimates from the literature and global OH fields from the GEOS Chemistry-Climate Model. Our analysis suggests these factors may have contributed a positive trend to [OH]_GLOBAL large enough to counter the decrease due to CH4.

Climate Change↗

NASA NTRS2014

A Computational and Experimental Study of Coflow Laminar Methane/Air Diffusion Flames: Effects of Fuel Dilution, Inlet Velocity, and Gravity

The influences of fuel dilution, inlet velocity, and gravity on the shape and structure of laminar coflow CH4-air diffusion flames were investigated computationally and experimentally. A series of nitrogen-diluted flames measured in the Structure and Liftoff in Combustion Experiment (SLICE) on board the International Space Station was assessed numerically under microgravity (mu g) and normal gravity (1g) conditions with CH4 mole fraction ranging from 0.4 to 1.0 and average inlet velocity ranging from 23 to 90 cm/s. Computationally, the MC-Smooth vorticity-velocity formulation was employed to describe the reactive gaseous mixture, and soot evolution was modeled by sectional aerosol equations. The governing equations and boundary conditions were discretized on a two-dimensional computational domain by finite differences, and the resulting set of fully coupled, strongly nonlinear equations was solved simultaneously at all points using a damped, modified Newton's method. Experimentally, flame shape and soot temperature were determined by flame emission images recorded by a digital color camera. Very good agreement between computation and measurement was obtained, and the conclusions were as follows. (1) Buoyant and nonbuoyant luminous flame lengths are proportional to the mass flow rate of the fuel mixture; computed and measured nonbuoyant flames are noticeably longer than their 1g counterparts; the effect of fuel dilution on flame shape (i.e., flame length and flame radius) is negligible when the flame shape is normalized by the methane flow rate. (2) Buoyancy-induced reduction of the flame radius through radially inward convection near the flame front is demonstrated. (3) Buoyant and nonbuoyant flame structure is mainly controlled by the fuel mass flow rate, and the effects from fuel dilution and inlet velocity are secondary.

flames↗

NASA NTRS2014

The Gemini NICI Planet-Finding Campaign: The Offset Ring of HR 4796 A

We present J, H, CH4 short (1.578 micrometers), CH4 long (1.652 micrometers) and K(sub s)-band images of the dust ring around the 10 Myr old star HR 4796 A obtained using the Near Infrared Coronagraphic Imager (NICI) on the Gemini-South 8.1 m Telescope. Our images clearly show for the first time the position of the star relative to its circumstellar ring thanks to NICI's translucent focal plane occulting mask. We employ a Bayesian Markov chain Monte Carlo method to constrain the offset vector between the two. The resulting probability distribution shows that the ring center is offset from the star by 16.7 +/- 1.3 milliarcseconds along a position angle of 26 +/- 3deg, along the PA of the ring, 26.47 +/- 0.04deg. We find that the size of this offset is not large enough to explain the brightness asymmetry of the ring. The ring is measured to have mostly red reflectivity across the JHKs filters, which seems to indicate micron-sized grains. Just like Neptune's 3:2 and 2:1 mean-motion resonances delineate the inner and outer edges of the classical Kuiper belt, we find that the radial extent of the HR 4796 A and the Fomalhaut rings could correspond to the 3:2 and 2:1 mean-motion resonances of hypothetical planets at 54.7 AU and 97.7 AU in the two systems, respectively. A planet orbiting HR 4796 A at 54.7 AU would have to be less massive than 1.6 Jup mass so as not to widen the ring too much by stirring.

Near Infrared Coronagraphic Imager (NICI)↗

NASA NTRS2016

Pluto and Charon: Surface Colors and Compositions - A Hypothesis

The surface of Pluto displays an array of colors ranging from yellow to red to brown, while the surface of Charon is largely gray with a north polar zone of red color similar to regions on Pluto. Pluto's surface shows layers of intensely colored material in tilted and transported blocks, and fractured geo-graphical units. This arrangement suggests episodes of formation or deposition of that material interspersed with episodes of emplacement of ices having little or no color. The ices identified on the surfaces of these two bodies (N2, CH4, CO, C2H6, H2O on Pluto, and H2O and NH3 on Charon) are colorless, as are nearly all ices in a powdery state. The colors on Pluto probably arise from the in situ formation of a macro-molecular carbonaceous material generated by energetic processing of the ices on the surface. Laboratory experiments producing refractory tholins particularly relevant to Pluto explored the chemistry of both UV and low-energy electron bombardment of a mix of Pluto ices (N2:CH4:CO = 100:1:1). We can term this Pluto ice tholin PIT. Water ice in the crystalline state characterizes Charon's surface, and while most of Charon's surface is neutral in color, with geometric albedo approximately 0.38, the polar zone and a light cover of fainter but similar reddish color over some surface regions suggest a common origin with the colored material on Pluto. NH3 or NH3 x nH2O was identified from disk-integrated Earth-based spectra, and a few concentrated NH3 exposures have been found in the New Horizons spectral images.

Pluto↗

NASA NTRS2016

Tholins as Coloring Agents on Pluto and Other Icy Solar System Bodies

Tholins are refractory organic solids of complex structure and high molecular weight, with a wide range of color ranging from yellow and orange to dark red, and through tan to black. They are made in the laboratory by energy deposition (photons or charged particles) in gases and ices containing the simple molecules (e.g., N2, CH4, CO) found in planetary atmospheres or condensed on planetary surfaces. They are widely implicated in providing the colors and albedos, particularly in the region 0.3-1.0 microns, of several outer Solar System bodies, including Pluto, as well as aerosols in planetary atmospheres such as Titan. Recent color images of Pluto with the New Horizons spacecraft show concentrations of coloring agent(s) in some regions of the surface, and apparent near-absence in other regions. Tholins that may to some degree represent surface chemistry on Pluto have been synthesized in the laboratory by energetic processing of mixtures of the ices (N2, CH4, CO) known on Pluto's surface, or the same molecules in the gas phase. Details of the composition and yield vary with experimental conditions. Chemical analysis of Pluto ice tholins shows evidence of amides, carboxylic acids, urea, carbodiimides, and nitriles. Aromatic/olefinic, amide, and other functional groups are identified in XANES analysis. The ice tholins produced by e- irradiation have a higher concentration of N than UV ice tholins, with N/C approx. 0.9 (versus approx. 0.5 for UV tholins) and O/C approx.0.2. Raman spectra of the electron tholin show a high degree of structural disorder, while strong UV fluorescence indicates a large aromatic content. EUV photolysis of a Pluto gaseous atmosphere analog yields pale yellow solids relatively transparent in the visual, and with aliphatic CH bonds prominent in IR spectra. This or similar material may be responsible for Pluto's hazes.

Tholins↗

NASA NTRS2016

En Route to Destruction: the Evolution in Composition of Ices in Comet D 2012 S1 (ISON) Between 1.2 and 0.34 Au from the Sun as Revealed at Infrared Wavelengths

We report production rates for H2O and eight trace molecules (CO, C2H6, CH4, CH3OH, NH3, H2CO, HCN, C2H2) in the dynamically new, Sun-grazing Comet C2012 S1 (ISON), using high-resolution spectroscopy at Keck II and the NASA IRTF on 10pre-perihelion dates encompassing heliocentric distances Rh1.210.34 AU. Measured water production rates spanned two orders of magnitude, consistent with a long-term heliocentric power law Q(H2O) Rh-3.10.1). Abundance ratios for CO, C2H6, and CH4 with respect to H2O remained constant with Rh and below their corresponding mean values measured among a dominant sample of Oort Cloud comets. CH3OH was also depleted for Rh 0.5 AU, but was closer to its mean value for Rh0.5 AU. The remaining four molecules exhibited higher abundance ratios within 0.5 AU: for Rh 0.8 AU, NH3 and C2H2 were consistent with their mean values while H2CO and HCN were depleted. For Rh 0.5 AU, all four were enriched, with NH3, H2CO, and HCN increasing most. Spatial profiles of gas emission in ISON consistently peaked sunward of the dust continuum, which was asymmetric antisunward and remained singly peaked for all observations. NH3 within 0.5 AU showed a broad spatial distribution, possibly indicating its release in the coma provided that optical depth effects were unimportant. The column abundance ratio NH2H2O at 0.83 AU was close to the typical NHOH from optical wavelengths, but was higher within 0.5 AU. Establishing its production rate and testing its parentage (e.g., NH3) require modeling of coma outflow.

Disanti, M. A.↗

NASA NTRS2017

Methane Measurements from Space: Technical Challenges and Solutions

We report on an airborne demonstration of atmospheric methane (CH4) measurements with an Integrated Path Differential Absorption (IPDA) lidar using an optical parametric oscillator (OPO) and optical parametric amplifier (OPA) laser transmitter and a sensitive avalanche photo detector. The lidar measures the CH4 absorption at multiple, discrete wavelengths around 1650.9 nm. In September 2015, the instrument was deployed on NASAs DC-8 airborne laboratory and measured atmospheric methane over a wide range of topography and weather conditions from altitudes of 3 km to 13 km. In this paper, we will review the results from our flights, and identify areas of improvement.

lasers↗

NASA NTRS2017

Removal of Carbon Dioxide from Gas Mixtures Using Ion-Exchanged Silicoaluminophosphates

Na+-SAPO-34 sorbents were ion-exchanged with several individual metal cations for CO2 absorption at different temperatures (273-348 K) and pressures (<1 atm). In general, the overall adsorption performance of the exchanged materials increased as follows: Ce3+<Ti3+<Mg2+<Ca2+<Ag+<Na+<Sr2+. The strontium exchanged materials excelled at low-pressure ranges, exhibiting very sharp isotherms slopes at all temperatures. The Sr2+ species were responsible for the surface strong interaction and the cations were occupying exposed sites (SII') in the materials Chabazite cages. All the sorbent materials exhibited higher affinity for CO2 over the other gases tested (i.e., CH4, H2, N2 and O2) due to strong ion-quadrupole interactions. Sr2+-SAPO-34 sorbents are by far the best option for CO2 removal from CH4 mixtures, especially at low concentrations.

Hernandez-Maldonado, Arturo J↗

NASA NTRS2017

Titan Atmospheric Entry Radiative Heating

Detailed spectrally and spatially resolved radiance has been measured in the Electric Arc Shock Tube for conditions relevant to Titan entry, varying atmospheric composition, free-stream density (equivalent to altitude) and shock velocity. Permutations in atmospheric composition include 1.1, 2, 5 and 8.6 CH4 by mole with a balance of N2 and 1.5 CH4 0.5 Ar 98 N2 by mole, which is consistent with the current understanding of Titan's atmosphere. The effect of gas impurities identified in previous shock tube studies were also examined by testing in pure N2 and deliberate addition of air to the CH4N2 mixtures. The test campaign measured radiation at velocities from 4.7 kms to 8 kms and free-stream pressures from 0.1 to 0.47 Torr. These conditions cover a range of potential trajectories for flight missions, including a direct ballistic trajectory, a fly by or an extremely high speed entry. Radiances measured in this work are substantially larger compared to that reported both in past EAST test campaigns and other shock tube facilities. Depending on the metric used for comparison, the discrepancy can be as high as an order of magnitude. Potential causes for the discrepancy, such as the effect of oxygen due to Air leakage, gas composition and purity are discussed. The present work provides a new benchmark set of data to replace those published in previous studies.

Earth↗

NASA NTRS2017

Titan Atmospheric Entry Radiative Heating

Brandis, A. M↗

NASA NTRS2017

Organic Haze as a Biosignature in Anoxic Earth-Like Atmospheres

Early Earth may have hosted a biologically mediated global organic haze during the Archean eon (3.8-2.5 billion years ago). This haze would have significantly impacted multiple aspects of our planet, including its potential for habitability and its spectral appearance. Here, we model worlds with Archean-like levels of carbon dioxide orbiting the ancient Sun and anM4Vdwarf (GJ 876) and show that organic haze formation requires methane fluxes consistent with estimated Earth-like biological production rates. On planets with high fluxes of biogenic organic sulfur gases (CS2, OCS, CH3SH, and CH3SCH3), photochemistry involving these gases can drive haze formation at lower CH4/CO2 ratios than methane photochemistry alone. For a planet orbiting the Sun, at 30x the modern organic sulfur gas flux, haze forms at a CH4/CO2 ratio 20% lower than at 1x the modern organic sulfur flux. For a planet orbiting the M4V star, the impact of organic sulfur gases is more pronounced: at 1x the modern Earth organic sulfur flux, a substantial haze forms at CH4/CO2 approx. 0.2, but at 30x the organic sulfur flux, the CH4/CO2 ratio needed to form haze decreases by a full order of magnitude. Detection of haze at an anomalously low CH4/ CO2 ratio could suggest the influence of these biogenic sulfur gases and therefore imply biological activity on an exoplanet. When these organic sulfur gases are not readily detectable in the spectrum of an Earth-like exoplanet, the thick organic haze they can help produce creates a very strong absorption feature at UV-blue wavelengths detectable in reflected light at a spectral resolution as low as 10. In direct imaging, constraining CH4 and CO2 concentrations will require higher spectral resolution, and R > 170 is needed to accurately resolve the structure of the CO2 feature at 1.57 microns, likely the most accessible CO2 feature on an Archean-like exoplanet.

Arney, Giada↗

NASA NTRS2018

Stable Isotope Fractionation in Titan Aerosol Formation

Stable isotope ratio measurements are a powerful tool used to understand both ancient and modern planetary processes. Instruments on the Cassini- Huygens spacecraft along with ground-based observations have measured several isotope pairs, including C-13/C-12 and N-15/N-14, in Titan's atmosphere. This includes isotopic measurements of the major atmospheric species, CH4 and N2, along with HCN, HC3N, C2H2. C2H6 and C4H2. However, the isotopic fractionation of Titan's organic aerosol has not conclusively been measured and therefore the effect of aerosol formation as an isotopic fractionation pathway in Titan's atmosphere has not been considered. Laboratory studies have measured the carbon and/or nitrogen isotopic fractionation of Titan aerosol analogs. [18] found that the carbon fractionation of photochemical organic aerosol analogs are more enriched in C-13. This enrichment in the aerosol analogs is opposite of what is predicted for photochemical products by the kinetic isotope effect. Additionally, both [16] and [18] found that the nitrogen fractionation in the organic aerosol analogs are opposite of what is observed in Titan's atmospheric N2 and HCN, with the aerosol analogs being a light nitrogen sink. Here we monitor the gas phase during photochemical aerosol analog production as a function of reaction time. In a recirculation experiment, the isotopic fractionation of carbon within the gas-phase products is measured as the CH4 reservoir is depleted. This allows us to monitor the isotopic fractionation pathway during photochemical aerosol analog formation.

Ugelow, M. S.↗

NASA NTRS2018

Characterization of Wildfire Emissions in California: Analysis of Airborne Measurements of Trace Gases from 2013 to 2016

Biomass burning, which includes wildfires, prescribed, and agricultural fires, is an important source of trace gases and particles, and can influence air quality on a local, regional, and global scale. Biomass burning emissions are an important source of several key trace gases including carbon dioxide (CO2) and methane (CH4). With the threat of wildfire events increasing due to changes in land use, increasing population, and climate change, the importance of characterizing wildfire emissions is vital. In this work we characterize trace gas emissions from 9 wildfire events in California between 2013 – 2016, in some cases with multiple measurements performed during different burn periods of a specific wildfire. During this period airborne measurements of CO2, CH4, water vapor (H2O), ozone (O3), and formaldehyde (HCHO) were made by the Alpha Jet Atmospheric eXperiment (AJAX). Located in the Bay Area of California, AJAX is a joint effort between NASA Ames Research Center and H211, LLC. AJAX makes in-situ airborne measurements of trace gases 2-4 times per month, resulting in 229 flights to date since 2011. Results presented include emission ratios (ER) of trace gases measured by AJAX during fire flights, and comparisons of ERs are made for each fire, which differ in time, location, burning intensity, and fuel type. We also use our airborne measurements to compare with photochemical grid model results to assess model approximations of plume transport and chemical evolution from select wildfires.

Parworth, Caroline L.↗

NASA NTRS2019

Observation and Attribution of Temperature Trends near the Stratopause from HALOE

This study considers time series of temperature versus pressure, T(p), from the Halogen Occultation Experiment (HALOE) across the stratopause region, where the effects of radiative forcings from the greenhouse gases (CO2 and H2O) and from ozone are most pronounced. Trend analyses are from 1993-2005 for HALOE T(p) values at seven levels from 3.0 to 0.3 hPa with a vertical resolution of about 4 km and for eight latitude zones from 65°S to 65°N. The HALOE trends at 2.0 hPa are of the order of -1.0 K/decade across the tropics and subtropics, but then become smaller (-0.5 K/decade) at the middle latitudes. The near-global HALOE trend profile has a minimum cooling rate of -0.2 K/decade at 1.0 hPa, although it is more negative in the southern hemisphere and slightly positive in the northern hemisphere. The combined radiative forcings from CO2, H2O, and ozone are from -0.4 to -0.6 K/decade for 1993-2005 and are hemispherically symmetric. HALOE temperature trend and total radiative cooling profiles differ from those reported from observations and calculations for 1980-2000, mainly because the ozone trends changed from clearly negative in the 1980s through mid-1990s to slightly positive during the time of HALOE. Trends for the tracer, HALOE methane (CH4), increase from 2 to 4 %/decade from 50 hPa to 10 hPa, indicating an acceleration of the Brewer/Dobson circulation. Analyses of time series of CH4 across the stratopause reveal more variability in the northern hemisphere, where wave dissipation likely contributes to the heating.

Remsberg, Ellis↗

NASA NTRS2018

Quantifying Methane Leak Emissions by Fused Airborne Imaging Spectroscopy with in Situ Surface Mobile and Airborne Observations of a California Producing Oil Field

Methane (CH4) emission budgets remain uncertain and are projected to grow as oil and gas production from short-lived wells increases and their subsequent transport through aging gas distribution networks. Orders-of-magnitude variations in temporal, spatial, and emission scales present a key challenge to leak detection and quantification. Also, the probability distributions for large and stochastic, leaky systems such as geological reservoirs (by natural migration-seeps) and petroleum production from those reservoirs remain largely unknown, needed to address current approach limitations. The scale of many petroleum systems favors remote sensing, but the sensitivity of such systems often precludes detection of weak emissions. Consequently, an accurate evaluation requires that the relative contribution from the emission "tails" of small leaks also be quantified, which is best carried out using high-sensitivity in situ methods. Fusion of remote sensing and in situ approaches leverages complementary capabilities to address these limitations. We show results from mobile surface (AMOG) and airborne in situ (AJAX) and thermal-infrared (TIR) hyperspectral imaging spectroscopy (Mako) data applied to a producing oil field in the California Central Valley near Bakersfield. AMOG is an automobile-based mobile lab that measures 13 trace gases, aerosol size distributions and vertical profiles, 3D winds and other meteorology, and atmospheric column measurements by solar spectroscopy at highway speeds. AJAX measures 5 trace gases and 3D winds at ~140 m/s. Mako is a broad-area TIR imaging spectrometer that can discriminate multiple gases present in each pixel acquired. In situ-derived, total field emissions were 31±16 Gg/yr CH4. This was compared with Mako-derived emissions from all plumes identified across the study site. We found that super-emitters were not the dominant emissions mode and the spatial pattern of plume locations from production infrastructure was correlated to geological structures.

Leifer, Ira↗

NASA NTRS2018

Detection Opportunity for Aromatic Signature in Titan's Aerosols in the 4.1-5.3 μm Range

The Cassini/Huygens mission provided new insights on the chemistry of the upper atmosphere of Titan. The presence of large molecules and ions (>100's of amu) detected by Cassini at high altitude was not expected, and questions the original assumptions regarding the aerosol formation pathways. From recent laboratory studies, it has been shown that the inclusion of trace amounts of aromatic species drastically impacts the chemistry of aerosol formation and induces observable changes in the properties of the aerosols. In this Letter we focus on the effect of one of the simplest nitrogenous aromatics, pyridine (C5H5N), on the infrared signature of Titan's aerosol analogs. We introduce initial gas mixtures of (i) N2–C5H5N (100%/250 ppm), (ii) N2–CH4–C5H5N (99%/1%/250 ppm), and (iii) N2–CH4 (99%/1%) in a cold plasma discharge. The material produced, herein called tholins, is then analyzed by mid-infrared spectroscopy. When adding pyridine in the discharge, the tholins produced present an aromatic signature in the 4.1–5.3 μm (1850–2450 cm−1) spectral region, attributed to overtones of aromatic C–H out-of-plane bending vibrations. We also observe a spectral shift of the nitrile and iso-nitrile absorption band with the inclusion of pyridine in the gas mixture. These results could help to investigate the data obtained at Titan by the Cassini/Visual and Infrared Mapping Spectrometer (VIMS) instrument in the 1–5 μm infrared window.

Mathé, Christophe↗

NASA NTRSDate not supplied

Validation of the Aeroplanets Model in a Present-Day Earth Simulation

We present a validation of the Aeroplanets/Aerochemistry model (Gronoff et al. 2012; Airapetian et al. 2016), a one-dimensional photochemistry model, with another one-dimensional photochemistry model implemented in Hu et al. 2016. Results from a simulation of the atmosphere of present-day Earth from both models were used in the validation. Realistic initial conditions and concentrations were used in the validation, including surface emissions of CO, CH4, NH3, N2O, NO, SO2, OCS, H2S, and H2SO4. As part of the validation, we compare the vertical profile of concentration of key chemical species, including O3, N2O, NO, NO2, HNO3, HO2, OH, and CH4. Our model was able to create vertical concentration profiles of these species that closely matched the results from Hu et al. 2016. With the successful validation, we plan to use the Aeroplanets model to explore the role of ions and aerosols, formed the interaction of solar energetic particles and the atmosphere of early Earth, in generating key greenhouse gas species and gas species that support the formation of molecules crucial for life.

Bradley Michael Hegyi↗