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NASA NTRS1999

High-power continuous-wave mid-infrared radiation generated by difference frequency mixing of diode-laser-seeded fiber amplifiers and its application to dual-beam spectroscopy

We report the generation of up to 0.7 mW of narrow-linewidth (<60-MHz) radiation at 3.3 micrometers by difference frequency mixing of a Nd:YAG-seeded 1.6-W Yb fiber amplifier and a 1.5-micrometers diode-laser-seeded 0.6-W Er/Yb fiber amplifier in periodically poled LiNbO3. A conversion efficiency of 0.09%/W (0.47 mWW-2 cm-1) was achieved. A room-air CH4 spectrum acquired with a compact 80-m multipass cell and a dual-beam spectroscopic configuration indicates an absorption sensitivity of +/-2.8 x 10(-5) (+/-1 sigma), corresponding to a sub-parts-in-10(9) (ppb) CH4 sensitivity (0.8 ppb).

Non-NASA Center↗

NASA NTRS1987

Atmospheric H2O2 measurement: comparison of cold trap method with impinger bubbling method

Collection of atmospheric H2O2 was performed by a cold trap method using dry ice-acetone as the refrigerant. The air was drawn by a pump into a glass gas trap immersed in the dry ice-acetone slush in a dewar flask at a flow rate of 2.5 l min-1 for approximately 2 h. Collection efficiency was > 99% and negligible interferences by O3, SO2 or organic matter with the collected H2O2 in the trap were observed. This method was compared with the air impinger bubbling method which has been previously described (Kok et al., 1978a, b, Envir. Sci. Technol. 12, 1072-1080). The measured total peroxide (H2O2 + organic peroxide) values in a series of aim samples collected by the impinger bubbling method (0.06-3.7 ppb) were always higher than those obtained by the cold trap method (0.02-1.2 ppb). Laboratory experiments suggest that the difference in values between the two methods probably results from the aqueous phase generation of H2O2 and organic peroxide in the impinger solution by a reaction of atmospheric O3 with olefinic and aromatic compounds. If these O3-organic compound reactions which occur in the impinger also occur in aqueous droplets in the atmosphere, the process could be very important for aqueous phase generation of H2O2 in clouds and rainwater.

NASA Discipline Exobiology↗

NASA NTRS1997

Fullerenes, fulleranes and polycyclic aromatic hydrocarbons in the Allende meteorite

In this paper, we confirm our earlier observations of fullerenes (C60 and C70) in the Allende meteorite (Becker et al., 1994a, 1995). Fullerene C60 was also detected in two separate C-rich (approximately 0.5-1.0%) dark inclusions (Heymann et al., 1987) that were hand picked from the Allende sample. The amounts of C60 detected were approximately 5 and approximately 10 ppb, respectively, which is considerably less than what was detected in the Allende 15/21 sample (approximately 100 ppb; Becker et al., 1994a, 1995). This suggests that fullerenes are heterogeneously distributed in the meteorite. In addition, we present evidence for fulleranes, (C60Hx), detected in separate samples by laser desorption (reflectron) time-of-flight (TOF) mass spectrometry (LDMS). The LDMS spectra for the Allende extracts were remarkably similar to the spectra generated for the synthetic fullerane mixtures. Several fullerane products were synthesized using a Rh catalyst (Becker et al., 1993a) and separated using high-performance liquid chromatography (HPLC). Polycyclic aromatic hydrocarbons (PAHs) were also observed ppm levels) that included benzofluoranthene and corannulene, a cup-shaped molecule that has been proposed as a precursor molecule to the formation of fullerenes in the gas phase (Pope et al., 1993).

NASA Center ARC↗

NASA NTRS1993

Ion mobility spectrometry of hydrazine, monomethylhydrazine, and ammonia in air with 5-nonanone reagent gas

Hydrazine (HZ) and monomethylhydrazine (MMH) in air were monitored continuously using a hand-held ion mobility spectrometer equipped with membrane inlet, 63Ni ion source, acetone reagent gas, and ambient temperature drift tube. Response characteristics included detection limit, 6 ppb; linear range, 10-600 ppb; saturated response, >2 ppm; and stable response after 15-30 min. Ammonia interfered in hydrazines detection through a product ion with the same drift time as that for MMH and HZ. Acetone reagent gas was replaced with 5-nonanone to alter drift times of product ions and separate ammonia from MMH and HZ. Patterns in mobility spectra, ion identifications from mass spectra, and fragmentation cross-sections from collisional-induced dissociations suggest that drift times are governed by ion-cluster equilibria in the drift region of the mobility spectrometer. Practical aspects including calibration, stability, and reproducibility are reported from the use of a hand-held mobility spectrometer on the space shuttle Atlantis during mission STS-37.

Flight Experiment↗

NASA NTRS2001

Global Modeling of Tropospheric Chemistry with Assimilated Meteorology: Model Description and Evaluation

We present a first description and evaluation of GEOS-CHEM, a global three-dimensional (3-D) model of tropospheric chemistry driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Data Assimilation Office (DAO). The model is applied to a 1-year simulation of tropospheric ozone-NOx-hydrocarbon chemistry for 1994, and is evaluated with observations both for 1994 and for other years. It reproduces usually to within 10 ppb the concentrations of ozone observed from the worldwide ozonesonde data network. It simulates correctly the seasonal phases and amplitudes of ozone concentrations for different regions and altitudes, but tends to underestimate the seasonal amplitude at northern midlatitudes. Observed concentrations of NO and peroxyacetylnitrate (PAN) observed in aircraft campaigns are generally reproduced to within a factor of 2 and often much better. Concentrations of HNO3 in the remote troposphere are overestimated typically by a factor of 2-3, a common problem in global models that may reflect a combination of insufficient precipitation scavenging and gas-aerosol partitioning not resolved by the model. The model yields an atmospheric lifetime of methylchloroform (proxy for global OH) of 5.1 years, as compared to a best estimate from observations of 5.5 plus or minus 0.8 years, and simulates H2O2 concentrations observed from aircraft with significant regional disagreements but no global bias. The OH concentrations are approximately 20% higher than in our previous global 3-D model which included an UV-absorbing aerosol. Concentrations of CO tend to be underestimated by the model, often by 10-30 ppb, which could reflect a combination of excessive OH (a 20% decrease in model OH could be accommodated by the methylchloroform constraint) and an underestimate of CO sources (particularly biogenic). The model underestimates observed acetone concentrations over the South Pacific in fall by a factor of 3; a missing source from the ocean may be implicated.

Bey, Isabelle↗

NASA NTRS1995

Aqueous nitrite ion determination by selective reduction and gas phase nitric oxide chemiluminescence

An improved method of flow injection analysis for aqueous nitrite ion exploits the sensitivity and selectivity of the nitric oxide (NO) chemilluminescence detector. Trace analysis of nitrite ion in a small sample (5-160 microL) is accomplished by conversion of nitrite ion to NO by aqueous iodide in acid. The resulting NO is transported to the gas phase through a semipermeable membrane and subsequently detected by monitoring the photoemission of the reaction between NO and ozone (O3). Chemiluminescence detection is selective for measurement of NO, and, since the detection occurs in the gas-phase, neither sample coloration nor turbidity interfere. The detection limit for a 100-microL sample is 0.04 ppb of nitrite ion. The precision at the 10 ppb level is 2% relative standard deviation, and 60-180 samples can be analyzed per hour. Samples of human saliva and food extracts were analyzed; the results from a standard colorimetric measurement are compared with those from the new chemiluminescence method in order to further validate the latter method. A high degree of selectivity is obtained due to the three discriminating steps in the process: (1) the nitrite ion to NO conversion conditions are virtually specific for nitrite ion, (2) only volatile products of the conversion will be swept to the gas phase (avoiding turbidity or color in spectrophotometric methods), and (3) the NO chemiluminescence detector selectively detects the emission from the NO + O3 reaction. The method is free of interferences, offers detection limits of low parts per billion of nitrite ion, and allows the analysis of up to 180 microL-sized samples per hour, with little sample preparation and no chromatographic separation. Much smaller samples can be analyzed by this method than in previously reported batch analysis methods, which typically require 5 mL or more of sample and often need chromatographic separations as well.

NASA Discipline Environmental Health↗

NASA NTRS2008

Impact of Surface Emissions to the Zonal Variability of Tropical Tropospheric Ozone and Carbon Monoxide for November 2004

The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so called zonal 'wave-one' pattern, which is characterized by peak ozone concentrations (70-80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60-70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30-40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.

tropical tropospheric ozone↗

NASA NTRS2007

Mosaic-Detector-Based Fluorescence Spectral Imager

A battery-powered, pen-sized, portable instrument for measuring molecular fluorescence spectra of chemical and biological samples in the field has been proposed. Molecular fluorescence spectroscopy is among the techniques used most frequently in laboratories to analyze compositions of chemical and biological samples. Heretofore, it has been possible to measure fluorescence spectra of molecular species at relative concentrations as low as parts per billion (ppb), with a few nm spectral resolution. The proposed instrument would include a planar array (mosaic) of detectors, onto which a fluorescence spectrum would be spatially mapped. Unlike in the larger laboratory-type molecular fluorescence spectrometers, mapping of wavelengths to spatial positions would be accomplished without use of relatively bulky optical parts. The proposed instrument is expected to be sensitive enough to enable measurement of spectra of chemical species at relative concentrations <1 ppb, with spectral resolution that could be tailored by design to be comparable to a laboratory molecular fluorescence spectrometer. The proposed instrument (see figure) would include a button-cell battery and a laser diode, which would generate the monochromatic ultraviolet light needed to excite fluorescence in a sample. The sample would be held in a cell bounded by far-ultraviolet-transparent quartz or optical glass. The detector array would be, more specifically, a complementary metal oxide/ semiconductor or charge-coupled- device imaging photodetector array, the photodetectors of which would be tailored to respond to light in the wavelength range of the fluorescence spectrum to be measured. The light-input face of the photodetector array would be covered with a matching checkerboard array of multilayer thin film interference filters, such that each pixel in the array would be sensitive only to light in a spectral band narrow enough so as not to overlap significantly with the band of an adjacent pixel. The wavelength interval between adjacent pixels (and, thus, the spectral resolution) would typically be chosen by design to be approximately equal to the width of the total fluorescence wavelength range of interest divided by the number of pixels. The unitary structure comprising the photodetector array overlaid with the matching filter array would be denoted a hyperspectral mosaic detector (HMD) array.

Son, Kyung-Ah↗

NASA NTRS2011

A Hollow-Waveguide Gas Correlation Radiometer for Ultra-Precise Column Measurements of Formaldehyde on Mars

We present preliminary results in the development of a miniaturized gas correlation radiometer that implements a hollow-core optical fiber (hollow waveguide) gas correlation cell. The substantial reduction in mass and volume of the gas correlation cell makes this technology appropriate for an orbital mission -- capable of pinpointing sources of trace gases in the Martian atmosphere. Here we demonstrate a formaldehyde (H2CO) sensor and report a detection limit equivalent to approximately 30 ppb in the Martian atmosphere. The relative simplicity of the technique allows it to be expanded to measure a range of atmospheric trace gases of interest on Mars such as methane (CH4), water vapour (H2O), deuterated water vapour (HDO), and methanol (CH3OH). Performance of a formaldehyde instrument in a Mars orbit has been simulated assuming a 3 meter long, 1000 micron inner diameter hollow-core fiber gas correlation cell, a 92.8 degree sun-synchronous orbit from 400 km with a horizontal sampling scale of 10 km x 10 km. Initial results indicate that for one second of averaging, a detection limit of 1 ppb is possible.

Wilson, Emily L.↗

NASA NTRS2005

Precision Cryogenic Dilatometer

A dilatometer based on a laser interferometer is being developed to measure mechanical creep and coefficients of thermal expansion (CTEs) of materials at temperatures ranging from ambient down to 15 K. This cryogenic dilatometer has been designed to minimize systematic errors that limit the best previously available dilatometers. At its prototype stage of development, this cryogenic dilatometer yields a strain measurement error of 35 ppb or 1.7 ppb/K CTE measurement error for a 20-K thermal load, for low-expansion materials in the temperature range from 310 down to 30 K. Planned further design refinements that include a provision for stabilization of the laser and addition of a high-precision sample-holding jig are expected to reduce the measurement error to 5-ppb strain error or 0.3-ppb/K CTE error for a 20-K thermal load. The dilatometer (see figure) includes a common-path, differential, heterodyne interferometer; a dual-frequency, stabilized source bench that serves as the light source for the interferometer; a cryogenic chamber in which one places the material sample to be studied; a cryogenic system for cooling the interior of the chamber to the measurement temperature; an ultra-stable alignment stage for positioning the chamber so that the sample is properly positioned with respect to the interferometer; and a data-acquisition and control system. The cryogenic chamber and the interferometer portion of the dilatometer are housed in a vacuum chamber on top of a vibration isolating optical table in a cleanroom. The sample consists of two pieces a pillar on a base both made of the same material. Using reflections of the interferometer beams from the base and the top of the pillar, what is measured is the change in length of the pillar as the temperature in the chamber is changed. In their fundamental optical and electronic principles of operation, the laser light source and the interferometer are similar to those described in Common-Path Heterodyne Interferometers (NPO-20786), NASA Tech Briefs, Vol. 25, No. 7 (July 2001), page 12a, and Interferometer for Measuring Displacement to Within 20 pm (NPO- 21221), NASA Tech Briefs, Vol. 27, No. 7 (July 2003), page 8a. However, the present designs incorporate a number of special geometric, optical, and mechanical features to minimize optical and thermal-expansion effects that contribute to measurement errors. These features include the use of low-thermal expansion materials for structural components, kinematic mounting and symmetrical placement of optical components, and several measures taken to minimize spurious reflections of laser beams.

Dudik, Matthew↗

NASA NTRS2012

Scanning Laser Infrared Molecular Spectrometer (SLIMS)

This prototype innovation is a novel design that achieves very long, effective laser path lengths that are able to yield ppb (parts per billion) and sub-ppb measurements of trace gases. SLIMS can also accommodate multiple laser channels covering a wide range of wavelengths, resulting in detection of more chemicals of interest. The mechanical design of the mirror cell allows for the large effective path length within a small footprint. The same design provides a robust structure that lends itself to being immune to some of the alignment challenges that similar cells face. By taking a hollow cylinder and by cutting an elliptically or spherically curved surface into its inner wall, the basic geometry of a reflecting ring is created. If the curved, inner surface is diamond-turned and highly polished, a surface that is very highly reflective can be formed. The surface finish can be further improved by adding a thin chrome or gold film over the surface. This creates a high-quality, curved, mirrored surface. A laser beam, which can be injected from a small bore hole in the wall of the cylinder, will be able to make many low-loss bounces around the ring, creating a large optical path length. The reflecting ring operates on the same principle as the Herriott cell. The difference exists in the mirror that doesn't have to be optically aligned, and which has a relatively large, internal surface area that lends itself to either open air or evacuated spectroscopic measurements. This solid, spherical ring mirror removes the possibility of mirror misalignment caused by thermal expansion or vibrations, because there is only a single, solid reflecting surface. Benefits of the reflecting ring come into play when size constraints reduce the size of the system, especially for space missions in which mass is at a premium.

Scott, David C.↗

NASA NTRS2013

Investigating the Origin of Chlorohydrocarbons Detected by the Sample Analysis at Mars (SAM) Instrument at Rocknest

The search for organic compounds on Mars, including molecules of either abiotic or biological origin is one of the key goals of the Mars Science Laboratory (MSL) mission. Previously the Viking and Phoenix Lander missions searched for organic compounds, but did not find any definitive evidence of martian organic material in the soils. The Viking pyrolysis gas chromatography mass spectrometry (GCMS) instruments did not detect any organic compounds of martian or exogenous origin above a level of a few parts-per-billion (ppb) in the near surface regolith at either landing site [1]. Viking did detect chloromethane and dichloromethane at pmol levels (up to 40 ppb) after heating the soil samples up to 500 C (Table 1), although it was originally argued that the chlorohydrocarbons were derived from cleaning solvents used on the instrument hardware, and not from the soil samples themselves [1]. More recently, it was suggested that the chlorohydrocarbons detected by Viking may have been formed by oxidation of indigenous organic matter during pyrolysis of the soil in the presence of perchlorates [2]. Although it is unknown if the Viking soils contained perchlorates, Phoenix did reveal relatively high concentrations (~0.6 wt%) of perchlorate salt in the icy regolith [3], therefore, it is possible that the chlorohydrocarbons detected by Viking were produced, at least partially, during the experiments [2,4]. The Sample Analysis at Mars (SAM) instrument suite on MSL analyzed the organic composition of the soil at Rocknest in Gale Crater using a combination of pyrolysis evolved gas analysis (EGA) and GCMS. One empty cup procedural blank followed by multiple EGA-GCMS analyses of the Rocknest soil were carried out. Here we will discuss the results from these SAM measurements at Rocknest and the steps taken to determine the source of the chlorohydrocarbons.

Glavin, D.↗

NASA NTRS2004

A Portable Electronic Nose For Hydrazine and Monomethyl Hydrazine Detection

The Space Program and military use large quantities Hydrazine (Hz) and monomethyl hydrazine (MMI-I) as rocket propellant. These substances are very toxic and are suspected human carcinogens. The American Conference of Governmental Industrial Hygienist set the threshold limit value to be 10 parts per billion (ppb). Current off-the-shelf portable instruments require 10 to 20 minutes of exposure to detect 10 ppb concentration. This shortcofriing is not acceptable for many operations. A new prototype instrument using a gas sensor array and pattern recognition software technology (i.e., an electronic nose) has demonstrated the ability to identify either Hz or MM}{ and quantify their concentrations at 10 parts per billion in 90 seconds. This paper describes the design of the portable electronic nose (e-nose) instrument, test equipment setup, test protocol, pattern recognition algorithm, concentration estimation method, and laboratory test results.

Young, Rebecca C.↗

NASA NTRS2013

Evaluation of ACCMIP Outgoing Longwave Radiation from Tropospheric Ozone Using TES Satellite Observations.

We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5-20 ppb) in the Southern Hemisphere (SH) and modest high bias (5-10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005-2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120mW/ sq. m OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39+/- 41mW/ sq. m relative to TES data. We show that there is a correlation (Sq. R = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750-2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100mW/ sq. m. Removing these models leads to a mean ozone radiative forcing of 394+/- 42mW/ sq. m. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 +/- 60mW/ sq. m derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

troposphere↗

NASA NTRS2016

Silver Ion Biocide Delivery System for Water Disinfection

U.S. space exploration missions have long considered returning to the Moon and exploration of Mars that challenge life support systems. For these long duration missions, there is interest in replacing the iodine water treatment system with ionic silver, a proven biocide. For long duration exploration missions, it is imperative that an effective biocide be used that prevents microbial growth, biofilm formation, and microbially induced corrosion in the water storage and distribution systems while minimizing logistical supply requirements associated with the biocide delivery system. Two biocide delivery systems have been developed that electrochemically produce silver ions for disinfecting water throughout the water storage and distribution system. One system uses a newly developed hybrid micro-filtration and ion-exchange membrane to produce an abundance of silver ions at the 1000 ppb level upstream in the water distribution system to prevent biofilm growth. This is followed by a downstream collection module that electrochemically removes these silver ions before the water is discharged. Another approach uses a membraneless reactor to produce a 1000 ppb silver ion concentration level that also has a mechanically driven electrode cleaning mechanism that removes oxide films ensuring long life operation. By maintaining a sufficiently high level of silver ions throughout the water storage and distribution system, biofilm formation is suppressed. This approach overcomes present concerns where spurious silver deposition occurs on the container and flow line surfaces thus lowering the silver ion concentration to unsatisfactory disinfection levels.

Slote, Benjamin M.↗

NASA NTRS2016

Analysis of Summer-Time Ozone and Precursor Species in the Southeast United States

Ozone (O3) is a greenhouse gas and toxic pollutant which plays a major role in air quality and atmospheric chemistry. The understanding and ability to model the horizontal and vertical structure of O3 mixing ratios is difficult due to the complex formation/destruction processes and transport pathways that cause large variability of O3. The Environmental Protection Agency has National Ambient Air Quality Standards for O3 set at 75 ppb with future standards proposed to be as low as 65 ppb. These lower values emphasize the need to better understand/simulate the transport processes, emission sources, and chemical processes controlling precursor species (e.g., NOx, VOCs, and CO) which influence O3 mixing ratios. The uncertainty of these controlling variables is particularly large in the southeast United States (US) which is a region impacted by multiple different emission sources of precursor species (anthropogenic and biogenic) and transport processes resulting in complex spatio-temporal O3 patterns. During this work we will evaluate O3 and precursor species in the southeast US applying models, ground-based and airborne in situ data, and lidar observations. In the summer of 2013, the UAH O3 Differential Absorption Lidar (DIAL) (part of the Tropospheric Ozone Lidar Network (TOLNet)) measured vertical O3 profiles from the surface up to approximately 12 km. During this period, the lidar observed numerous periods of dynamic temporal and vertical O3 structures. In order to determine the sources/processes impacting these O3 mixing ratios we will apply the CTM GEOS-Chem (v9-02) at a 0.25 deg x 0.3125 deg resolution. Using in situ ground-based (e.g., SEARCH Network, CASTNET), airborne (e.g., NOAA WP-3D - SENEX 2013, DC-8 - SEAC4RS), and TOLNet lidar data we will first evaluate the model to determine the capability of GEOS-Chem to simulate the spatio-temporal variability of O3 in the southeast US. Secondly, we will perform model sensitivity studies in order to quantify which emission sources (e.g., anthropogenic, biogenic, lighting, wildfire) and transport processes (e.g., stratospheric, long-range, local scale) are contributing to these TOLNet-observed dynamic O3 patterns. Results from the evaluation of the model and the study of sources/processes impacting observed O3 mixing ratios will be presented.

Optical Radar↗

NASA NTRS2017

Organic Matter in Extraterrestrial Water-Bearing Salt Crystals

Introduction: Direct samples of early Solar System fluids are present in two thermally-metamorphosed ordinary chondrite regolith breccias (Monahans (1998) [H5] and Zag [H3-6]), which were found to contain brine-bearing halite (NaCl) crystals that have been added to the regolith of an S-type asteroid following asteroidal metamorphism [1, 2]. The brine-bearing halite grains were proposed to be formed on an icy C-type asteroids (possibly Ceres), and transferred to an S-type asteroid via cryovolcanic event(s) [3]. A unique aspect of these halites is that they contain abundant organic rich solid inclusions hosted within the halites alongside the water inclusions. Methods: We analyzed in detail the compositions of the organic solids and the amino acid content of the halite crystals with two-step laser desorption/laser ionization mass spectrometry (L(sup 2) MS), Raman spectroscopy, X-ray absorption near edge structure (XANES), nanoscale secondary ion mass spectrometry (NanoSIMS), and ultra-performance liquid chromatography fluorescence detection and quadrupole time of flight hybrid mass spectrometry (UPLC-FD/QToF-MS). Results and Discussion: The L(sup 2) MS results show signatures of low-mass polyaromatic hydro-carbons (PAHs) indicated by sequences of peaks separated by 14 atomic mass units (amu) due to successive addition of methylene (CH2) groups to the PAH skeletons [4]. Raman spectra of the micron-sized solid inclusions of the halites indicate the presence of abundant and highly variable organic matter that include a mixture of short-chain aliphatic compounds and macromolecular carbon. C-XANES analysis identified C-rich areas with peaks at 285.0 eV (aromatic C=C) and 286.6 eV (vinyl-keto C=O). However, there is no 1s-sigma* exciton peak (291.7 eV) that is indicative of the development of graphene structure [5], which suggests the organics were synthesized cold. Na-noSIMS analyses show C-rich and N-rich areas that exhibit similar isotopic values with that of the IOM in the unweathered CR chondrites and less metamorphosed meteorites [6], and are moderately enriched in N-15 (delta N-15 = 106.1-164.5 per mille). The total amino acid distribution and abundance of the Zag matrix (approximately 1,940 parts per billion [ppb]) is comparable to other ordinary chondrites (60-3,330 ppb) [7, 8]. While the Zag matrix is gamma-ABA and EACA-deficient, the halite is shown to exhibit an opposite trend and is almost depleted in amino acids. The striking difference in the amino acid contents between the halite and matrix indicates their separate synthetic origins. Conclusion: Abundant, primitive, and highly-diverse N-15-rich organic compounds were detected in brine-water bearing halite crystals that were synthesized on a cryovolcanically-active asteroid. Our study suggests that the asteroidal parent body where the halite precipitated, potentially Ceres, is a host to abundance large variety organic precursors. Insoluble organic matter and amino acids can be synthesized from similar organic precusors under hydrous conditions [9].We envision that similar organic synthetic processes could have occurred on Ceres that synthesized organic solids as well as biologically relevant molecules.

Chan, Q. H. S.↗

NASA NTRS2016

Why Do Models Overestimate Surface Ozone in the Southeast United States?

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NO(x) triple bond NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC(exp 4)RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25 deg x 0.3125 deg horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NO(x) from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC(exp 4)RS observations of NO(x) and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NO(x) emissions from mobile and industrial sources must be reduced by 30-60%, dependent on the assumption of the contribution by soil NO(x) emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NO(x) emissions. We find that only half of isoprene oxidation proceeds by the high-NO(x) pathway to produce ozone; this fraction is only moderately sensitive to changes in NO(x) emissions because isoprene and NO(x) emissions are spatially segregated. GEOS-Chem with reduced NO(x) emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NO(x) oxidation products. However, the model is still biased high by 6 plus or minus 14 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.

Oxidation↗