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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS2002

Atmospheric pressure chemical ionization studies of non-polar isomeric hydrocarbons using ion mobility spectrometry and mass spectrometry with different ionization techniques

The ionization pathways were determined for sets of isomeric non-polar hydrocarbons (structural isomers, cis/trans isomers) using ion mobility spectrometry and mass spectrometry with different techniques of atmospheric pressure chemical ionization to assess the influence of structural features on ion formation. Depending on the structural features, different ions were observed using mass spectrometry. Unsaturated hydrocarbons formed mostly [M - 1]+ and [(M - 1)2H]+ ions while mainly [M - 3]+ and [(M - 3)H2O]+ ions were found for saturated cis/trans isomers using photoionization and 63Ni ionization. These ionization methods and corona discharge ionization were used for ion mobility measurements of these compounds. Different ions were detected for compounds with different structural features. 63Ni ionization and photoionization provide comparable ions for every set of isomers. The product ions formed can be clearly attributed to the structures identified. However, differences in relative abundance of product ions were found. Although corona discharge ionization permits the most sensitive detection of non-polar hydrocarbons, the spectra detected are complex and differ from those obtained with 63Ni ionization and photoionization. c. 2002 American Society for Mass Spectrometry.

Non-NASA Center↗
NASA NTRS1995

A new method for the preparation of polymeric porous layer open tubular columns for GC application

A new method to prepare polymeric PLOT columns by using in situ polymerization technology is described. The method involves a straightforward in situ polymerization of the monomer. The polymer produced is directly coated on the metal tubing. This eliminates many of the steps needed in conventional polymeric PLOT column preparation. Our method is easy to operate and produces very reproducible columns, as shown previously (T. C. Shen. J. Chromatogr. Sci. 30, 239, 1992). The effects of solvents, tubing pretreatments, initiators and reaction temperatures in the preparation of PLOT columns are studied. Several columns have been developed to separate (1) highly polar compounds, such as water and ammonia or water and HCN, and (2) hydrocarbons and inert gases. A recent improvement has allowed us to produce bonded polymeric PLOT columns. These were studied, and the results are included also.

NASA Discipline Exobiology↗
NASA NTRS1997

HCO+ in the coma of comet Hale-Bopp

Maps of comet C/1995 O1 (Hale-Bopp) in the millimeter-wave emission of the ion HCO+ revealed a local minimum near the nucleus position, with a maximum about 100,000 km in the antisolar direction. These observed features of the HCO+ emission require a low abundance of HCO+ due to enhanced destruction in the inner coma of the comet, within a region of low electron temperature (Te). To set constraints on the formation of HCO+ in the coma, as well as the location and magnitude of the transition to higher Te, the data are compared with the results of ion-molecule chemistry models.

Non-NASA Center↗
NASA NTRS1999

Envelope structure of deeply embedded young stellar objects in the Serpens Molecular Cloud

Aperture-synthesis and single-dish (sub-) millimeter molecular-line and continuum observations reveal in great detail the envelope structure of deeply embedded young stellar objects (SMM 1 = FIRS 1, SMM 2, SMM 3, SMM 4) in the densely star-forming Serpens Molecular Cloud. SMM 1, 3, and 4 show partially resolved (>2" = 800 AU) continuum emission in the beam of the Owens Valley Millimeter Array at lambda = 3.4-1.4 mm. The continuum visibilities accurately constrain the density structure in the envelopes, which can be described by a radial power law with slope -2.0 +/- 0.5 on scales of 300 to 8000 AU. Inferred envelope masses within a radius of 8000 AU are 8.7, 3.0, and 5.3 Msolar for SMM 1, 3, and 4, respectively. A point source with 20%-30% of the total flux at 1.1 mm is required to fit the observations on long baselines, corresponding to warm envelope material within approximately 100 AU or a circumstellar disk. No continuum emission is detected interferometrically toward SMM 2, corresponding to an upper limit of 0.2 Msolar assuming Td = 24 K. The lack of any compact dust emission suggests that the SMM 2 core does not contain a central protostar. Aperture-synthesis observations of the 13CO, C18O, HCO+, H13CO+, HCN, H13CN, N2H+ 1-0, SiO 2-1, and SO 2(2)-1(1) transitions reveal compact emission toward SMM 1, 3, and 4. SMM 2 shows only a number of clumps scattered throughout the primary field of view, supporting the conclusion that this core does not contain a central star. The compact molecular emission around SMM 1, 3, and 4 traces 5"-10" (2000-4000 AU) diameter cores that correspond to the densest regions of the envelopes, as well as material directly associated with the molecular outflow. Especially prominent are the optically thick HCN and HCO+ lines that show up brightly along the walls of the outflow cavities. SO and SiO trace shocked material, where their abundances may be enhanced by 1-2 orders of magnitude over dark-cloud values. A total of 31 molecular transitions have been observed with the James Clerk Maxwell and Caltech Submillimeter telescopes in the 230, 345, 490, and 690 GHz atmospheric windows toward all four sources, containing, among others, lines of CO, HCO+, HCN, H2CO, SiO, SO, and their isotopomers. These lines show 20-30 km s-1 wide line wings, deep and narrow (1-2 km s-1) self-absorption, and 2-3 km s-1 FWHM line cores. The presence of highly excited lines like 12CO 4-3 and 6-5, 13CO 6-5, and several H2CO transitions indicates the presence of material with temperatures > or approximately 100 K. Monte Carlo calculations of the molecular excitation and line transfer show that the envelope model derived from the dust emission can successfully reproduce the observed line intensities. The depletion of CO in the cold gas is modest compared to values inferred in objects like NGC 1333 IRAS 4, suggesting that the phase of large depletions through the entire envelope is short lived and may be influenced by the local star formation density. Emission in high-excitation lines of CO and H2CO requires the presence of a small amount of approximately 100 K material, comprising less than 1% of the total envelope mass and probably associated with the outflow or the innermost region of the envelope. The derived molecular abundances in the warm (Tkin > 20 K) envelope are similar to those found toward other class 0 YSOs like IRAS 16293-2422, though some species appear enhanced toward SMM 1. Taken together, the presented observations and analysis provide the first comprehensive view of the physical and chemical structure of the envelopes of deeply embedded young stellar objects in a clustered environment on scales between 1000 and 10,000 AU.

NASA Discipline Exobiology↗
NASA NTRS1999

The interstellar 4.62 micron band

We present new 4.5-5.1 micron (2210-1970 cm-1) spectra of embedded protostars, W33 A, AFGL 961 E, AFGL 2136, NGC 7538 IRS 9, and Mon R2 IRS 2, which contain a broad absorption feature located near 4.62 micron (2165 cm-1), commonly referred to in the literature as the "X-C triple bond N" band. The observed peak positions and widths of the interstellar band agree to within 2.5 cm-1 and 5 cm-1, respectively. The strengths of the interstellar 4.62 micrometers band and the ice absorption features in these spectra are not correlated, which suggests a diversity of environmental conditions for the ices we are observing. We explore several possible carriers of the interstellar band and review possible production pathways through far-ultraviolet photolysis (FUV), ion bombardment of interstellar ice analog mixtures, and acid-base reactions. Good fits to the interstellar spectra are obtained with an organic residue produced through ion bombardment of nitrogen-containing ices or with the OCN- ion produced either through acid-base reactions or FUV photolysis of NH3-containing ices.

NASA Center ARC↗
NASA NTRS1995

Geochemical characteristics of organic compounds in a permafrost sediment core sample from northeast Siberia, Russia

We studied total organic carbon (TOC), hydrocarbons and fatty acids in a permafrost sediment core sample (well 6-90, length 32.0 m, 1.5-2.5 Ma BP) from northeast Siberia (approximately 70 degrees N, 158 degrees E), Russia, to elucidate their geochemical features in relation to source organisms and paleoenvironmental conditions. Long-chain n-alkanes and n-alkanoic acids (>C19) were most predominant hydrocarbons and fatty acids, respectively, so organic matter in the sediment core was derived mainly from vascular plants and, to a much smaller extent, from bacteria. Low concentrations of unsaturated fatty acids revealed that organic matter in the sediment core was considerably degraded during and/or after sedimentation. The predominance of vascular plant components, the major ionic components of nonmarine sources, and geological data strongly implied that the sediment layers were formed in shallow lacustrine environments, such as swamp with large influences of tundra or forest-tundra vegetation. Also, no drastic changes in paleoenvironmental conditions for biological activity or geological events, such as sea transgressions or ice-sheet influences, occurred at the sampling site approximately 100 km from the coast of the East Siberian Sea during the late Pliocene an early Pleistocene periods.

NASA Discipline Exobiology↗
NASA NTRS1996

Phenols in hydrothermal petroleums and sediment bitumen from Guaymas Basin, Gulf of California

The aliphatic, aromatic and polar (NSO) fractions of seabed petroleums and sediment bitumen extracts from the Guaymas Basin hydrothermal system have been analyzed by gas chromatography and gas chromatography-mass spectrometry (free and silylated). The oils were collected from the interiors and exteriors of high temperature hydrothermal vents and represent hydrothermal pyrolyzates that have migrated to the seafloor by hydrothermal fluid circulation. The downcore sediments are representative of both thermally unaltered and thermally altered sediments. The survey has revealed the presence of oxygenated compounds in samples with a high degree of thermal maturity. Phenols are one class of oxygenated compounds found in these samples. A group of methyl-, dimethyl- and trimethyl-isoprenoidyl phenols (C27-C29) is present in all of the seabed NSO fractions, with the methyl- and dimethyl-isoprenoidyl phenols occurring as major components, and a trimethyl-isoprenoidyl phenol as a minor component. A homologous series of n-alkylphenols (C13-C33) has also been found in the seabed petroleums. These phenols are most likely derived from the hydrothermal alteration of sedimentary organic matter. The n-alkylphenols are probably synthesized under hydrothermal conditions, but the isoprenoidyl phenols are probably hydrothermal alteration products of natural product precursors. The suites of phenols do not appear to be useful tracers of high temperature hydrothermal processes.

Non-NASA Center↗
NASA NTRS1996

The IRS 1 circumstellar disk, and the origin of the jet and CO outflow in B5

We report the discovery of the inner edge of the high velocity CO outflow associated with the bipolar jet originating from IRS 1 in Barnard 5 and the first ever resolution of its circumstellar disk in the 2.6 mm dust continuum and C18O. From high spatial resolution observations made with the Owens Valley Millimeter Array we are able to locate the origin of the outflow to within approximately 500 AU on either side of IRS 1 and apparently at the edge of, or possibly within, its circumstellar disk. The orientation of the continuum disk is perpendicular to the highly collimated jet outflow recently seen in optical emission at much farther distances. The disk has been detected in C18O giving a disk mass approximately 0.16 M (solar). Our HCO+ and HCN maps indicate significant chemical differentiation in the circumstellar region on small scales with HCO+ tracing an extended disk of material. The 12CO interferometer maps of the outflow show two conelike features originating at IRS 1, the blue one fanning open to the northeast and the red one to the southwest. The vertices of the cones are on either side of the circumstellar disk and have a projected opening angle of about 90 degrees. The intrinsic opening angle is in the range of 60 degrees-90 degrees which leads to significant interaction between outflow and infall.

NASA Center JPL↗
NASA NTRS1997

Chemical and physical gradients along the OMC-1 ridge

We present a survey of the distribution of 20 chemical and isotopic molecular species along the central ridge of the Orion molecular cloud from 6' north to 6' south of BN-KL observed with the QUARRY focal plane array on the FCRAO 14 m telescope, which provides an angular resolution of approximately 50" in the 3 mm wavelength region. We use standard tools of multivariate analysis for a systematic investigation of the similarities and differences among the maps of integrated intensities of the 32 lines observed. The maps fall in three broad classes: first, those strongly peaked toward BN-KL; second, those having rather flat distributions along the ridge; and third, those with a clear north-south gradient or contrast. We identify six positions or regions where we calculate relative abundances. Line velocities and line widths indicate that the optically thin lines generally trace the same volume of dense gas, except in the molecular bar, where C18O, C34S, H13CO+, CN, C2H, SO, and C3H2 have velocities characteristic of the bar itself, whereas the emission from other detected species is dominated by the background cloud. The strongest abundance variations in our data are the well-known enhancements seen in HCN, CH3OH, HC3N, and SO toward BN-KL and, less strongly, toward the Orion-South outflow 1'.3S. The principal result of this study is that along the extended quiescent ridge the chemical abundances, within factors of 3-4, exhibit an impressive degree of uniformity. The northern part of the ridge has a chemistry closest to that found in quiescent dense clouds. While temperature and density are similar around the northern radical-ion peak near 3'.5N and in the southern core near 4'.2S, some abundances, in particular, those of the ions HCO+ and N2H+, are significantly lower toward 4'.2S. The areas near 4.'2S and the molecular bar itself around (1'.7E, 2'.4S) stand out with peculiar and similar properties probably caused by stronger UV fields penetrating deeper into the clumpy molecular gas. This leads to higher electron abundances and thereby reduced abundances of the ions, as well as a lack of complex molecules.

NASA Discipline Exobiology↗
NASA NTRS1986

Biological marker distribution in coexisting kerogen, bitumen and asphaltenes in Monterey Formation diatomite, California

Organic-rich (18.2%) Monterey Formation diatomite from California was studied. The organic matter consist of 94% bitumen and 6% kerogen. Biological markers from the bitumen and from pyrolysates of the coexisting asphaltenes and kerogen were analyzed in order to elucidate the relationship between the various fractions of the organic matter. While 17 alpha(H), 18 alpha(H), 21 alpha(H)-28,30-bisnorhopane was present in the bitumen and in the pryolysate of the asphaltenes, it was not detected in the pyrolysates of the kerogen. A C40-isoprenoid with "head to head" linkage, however, was present in pyrolysates of both kerogen and asphaltenes, but not in the bitumen from the diatomite. The maturation level of the bitumen, based on the extent of isomerization of steranes and hopanes, was that of a mature oil, whereas the pyrolysate from the kerogen showed a considerably lower maturation level. These relationships indicate that the bitumen may not be indigenous to the diatomite and that it is a mature oil that migrated into the rock. We consider the possibility, however, that some of the 28,30-bisnorhopane-rich Monterey Formation oils have not been generated through thermal degradation of kerogen, but have been expelled from the source rock at an early stage of diagenesis.

Non-NASA Center↗
NASA NTRS1995

Laboratory comparisons of organic materials to interstellar dust and the Murchison meteorite

Spectra of objects which lie along several lines of sight through the diffuse interstellar medium (DISM) reveal an absorption feature near 3.4 micrometers, which has been attributed to saturated aliphatic hydrocarbons on interstellar grains. The similarity of the absorption bands near 3.4 micrometers (2950 cm-1) along different lines of sight indicates that the carrier of this band lies in the diffuse dust. Several materials have been proposed as "fits" to the 3.4 micrometers feature over the years. A comparison of these identifications is presented. These comparisons illustrate the need for high resolution, high signal-to-noise observational data as a means of distinguishing between laboratory organics as matches to the interstellar material. Although any material containing hydrocarbons will produce features in the 3.4 micrometers region, the proposed "matches" to the DISM do differ in detail. These differences may help in the analyses of the chemical composition and physical processes which led to the production of the DISM organics, although ISO Observations through the 5-8 micrometers spectral region are essential for a definitive identification. A remarkable similarity between the spectrum of the diffuse dust and an organic extract from the Murchison meteorite suggests that some of the interstellar organic material may be preserved in primitive solar system bodies. The 3.4 micrometers absorption feature (in the rest frame) has recently been detected in external galaxies, indicating the widespread availability of organic material for incorporation into planetary systems.

NASA Center ARC↗
NASA NTRS1996

A search for HCCN in molecular clouds

We have conducted a deep search for HCCN towards the dark cloud TMC-l and several GMC's via its N(J) = 1(2)-->0(1) transition. HCCN was not detected in any of these sources. Towards TMC-l, assuming optically thin emission, the total column density upper limit is NHCCN < or = 2 x 10(12) cm-2, which corresponds to a fractional abundance upper limit with respect to molecular hydrogen of fHCCN < or = 2 x 10(-10). We find the abundance ratio of HCN:HCCN:HCCCN in TMC-l to be l : <0.01 : 0.3, which suggests that carbon-chain growth by the addition of single carbon atoms may not be efficient under dark cloud conditions. The HCCN abundance limit also places constraints on the branching ratio for the products of the dissociative electron recombination H3C2N+ + e.

Non-NASA Center↗
NASA NTRS1994

Evidence for only minor contributions from bacteria to sedimentary organic carbon

Because their molecular signatures are often prominent in extracts of sediments, bacteria are thought to be important contributors to petroleum source beds. It has been shown recently, however, that abundances of biomarkers do not always reflect relative contributions to sedimentary organic carbon (Corg). The contribution of photosynthetic green sulphur bacteria to sediments can be assessed effectively because the diagenetic products of distinctive carotenoids from these organisms occur widely and their biomass is isotopically labelled, being enriched in 13C. We show here that, although sediments and oils from the Western Canada and Williston basins contain prominent biomarkers of photosynthetic bacteria, the absence of 13C enrichment in the total Corg requires that the bacterial contribution is in fact minimal. Although the importance of bacterial reworking of sedimentary debris cannot be doubted, we argue that our findings, when considered in conjunction with those from other settings, suggest that bacterial biomass may commonly represent only a minor component of total Corg in carbonaceous rocks.

NASA Discipline Exobiology↗
NASA NTRS1996

A system and methodology for measuring volatile organic compounds produced by hydroponic lettuce in a controlled environment

A system and methodology were developed for the nondestructive qualitative and quantitative analysis of volatile emissions from hydroponically grown 'Waldmann's Green' leaf lettuce (Lactuca sativa L.). Photosynthetic photon flux (PPF), photoperiod, and temperature were automatically controlled and monitored in a growth chamber modified for the collection of plant volatiles. The lipoxygenase pathway products (Z)-3-hexenal, (Z)-3-hexenol, and (Z)-3-hexenyl acetate were emitted by lettuce plants after the transition from the light period to the dark period. The volatile collection system developed in this study enabled measurements of volatiles emitted by intact plants, from planting to harvest, under controlled environmental conditions.

NASA Discipline Life Support Systems↗
NASA NTRS1994

Isotopic analyses of nitrogenous compounds from the Murchison meteorite: ammonia, amines, amino acids, and polar hydrocarbons

The combined volatile bases (ammonia, aliphatic amines, and possibly other bases), ammonia, amino acids, and polar hydrocarbons were prepared from the Murchison meteorite for isotopic analyses. The volatile bases were obtained by cryogenic transfer after acid-hydrolysis of a hot-water extract and analyzed by combined gas chromatography-mass spectrometry of pentafluoropropionyl derivatives. The aliphatic amines present in this preparation comprise a mixture that includes both primary and secondary isomers through C5 at a total concentration of > or = 100 nmoles g-1. As commonly observed for meteoritic organic compounds, almost all isomers through C5 are present, and the concentrations within homologous series decrease with increasing chain length. Ammonia was chromatographically separated from the other volatile bases and found at a concentration of 1.1-1.3 micromoles g-1 meteorite. The ammonia analyzed includes contributions from ammonium salts and the hydrolysis of extractable organic compounds, e.g., carboxamides. Stable isotope analyses showed the volatile bases to be substantially enriched in the heavier isotopes, relative to comparable terrestrial compounds delta D < or = +1221%; delta 13C = +22%; delta 15N = +93%). Ammonia, per se, was found to have a somewhat lower delta 15N value (+69%) than the total volatile bases; consequently, a higher delta 15N (>93%) can be inferred for the other bases, which include the amines. Solvent-extractable polar hydrocarbons obtained separately were found to be enriched in 15N (delta 15N = +104%). Total amino acids, prepared from a hydrolyzed hot-water extract by cation exchange chromatography, gave a delta 15N of +94%, a value in good agreement with that obtained previously. Nitrogen isotopic data are also given for amino acid fractions separated chromatographically. The delta 15N values of the Murchison soluble organic compounds analyzed to date fall within a rather narrow range (delta 15N = +94 +/- 8%), an observation consistent with their formation, or formation of their precursors, by interstellar chemistry.

Non-NASA Center↗
NASA NTRS1995

Molecular indicators for palaeoenvironmental change in a Messinian evaporitic sequence (Vena del Gesso, Italy). II: High-resolution variations in abundances and 13C contents of free and sulphur-bound carbon skeletons in a single marl bed

The extractable organic matter of 10 immature samples from a marl bed of one evaporitic cycle of the Vena del Gesso sediments (Gessoso-solfifera Fm., Messinian, Italy) was analyzed quantitatively for free hydrocarbons and organic sulphur compounds. Nickel boride was used as a desulphurizing agent to recover sulphur-bound lipids from the polar and asphaltene fractions. Carbon isotopic compositions (delta vs PDB) of free hydrocarbons and of S-bound hydrocarbons were also measured. Relationships between these carbon skeletons, precursor biolipids, and the organisms producing them could then be examined. Concentrations of S-bound lipids and free hydrocarbons and their delta values were plotted vs depth in the marl bed and the profiles were interpreted in terms of variations in source organisms, 13 C contents of the carbon source, and environmentally induced changes in isotopic fractionation. The overall range of delta values measured was 24.7%, from -11.6% for a component derived from green sulphur bacteria (Chlorobiaceae) to -36.3% for a lipid derived from purple sulphur bacteria (Chromatiaceae). Deconvolution of mixtures of components deriving from multiple sources (green and purple sulphur bacteria, coccolithophorids, microalgae and higher plants) was sometimes possible because both quantitative and isotopic data were available and because either the free or S-bound pool sometimes appeared to contain material from a single source. Several free n-alkanes and S-bound lipids appeared to be specific products of upper-water-column primary producers (i.e. algae and cyanobacteria). Others derived from anaerobic photoautotrophs and from heterotrophic protozoa (ciliates), which apparently fed partly on Chlorobiaceae. Four groups of n-alkanes produced by algae or cyanobacteria were also recognized based on systematic variations of abundance and isotopic composition with depth. For hydrocarbons probably derived from microalgae, isotopic variations are well correlated with those of total organic carbon. A resistant aliphatic biomacromolecule produced by microalgae is, therefore, probably an important component of the kerogen. These variations reflect changes in the depositional environment and early diagenetic transformations. Changes in the concentrations of S-bound lipids induced by variations in conditions favourable for sulphurization were discriminated from those related to variations in primary producer assemblages. The water column of the lagoonal basin was stratified and photic zone anoxia occurred during the early and middle stages of marl deposition. During the last stage of the marl deposition the stratification collapsed due to a significant shallowing of the water column. Contributions from anaerobic photoautotrophs were apparently associated with variations in depth of the chemocline.

Non-NASA Center↗
NASA NTRS1995

Titan's stratospheric temperature asymmetry: a radiative origin?

During the 1981 Voyager encounter, Titan's stratosphere exhibited a large thermal asymmetry, with high northern latitudes being colder than comparable southern latitudes. Given the short radiative time constant, this asymmetry would not be expected at the season of the Voyager observations (spring equinox), if the infrared and solar opacity sources were distributed symmetrically. We have investigated the radiative budget of Titan's stratosphere, using two selections of Voyager IRIS spectra recorded at symmetric northern and southern latitudes. In the region 0.1-1 mbar, temperatures are 7 K colder at 50 degrees N than at 53 degrees S and the difference reaches approximately 13 K at 5 mbar. On the other hand, the northern region is strongly enriched in nitriles and hydrocarbons, and the haze optical depth derived from the continuum emission between 8 and 15 micrometers is twice as large as in the south. Cooling rate profiles have been computed at the two locations, using the gas and haze abundances derived from the IRIS measurements. We find that, despite lower temperatures, the cooling rate profiles in the pressure range 0.15-5 mbar are 20 to 40% larger in the north than in the south, because of the enhanced concentrations of infrared radiators. Because the northern hemisphere appears darker than the southern one in the Voyager images, enhanced solar heating is also expected to take place at 50 degrees N. Solar heating rate profiles have been calculated, with two different assumptions on the origin of the hemispheric asymmetry. In the most likely case where it results from a variation in the absorbance of the haze material, the heating rates are found to be 12-15% larger at the northern location than at the southern one, a smaller increase than that in the cooling rates. If the lower albedo in the north results from an increase in the particle number density, a 55 to 75% difference is found for the pressure range 0.15-5 mbar, thus larger than that calculated for the cooling rates. Considering the uncertainties in the haze model, dynamical heat transport may significantly contribute to the meridional temperature gradients observed in the stratosphere. On the other hand, the latitudinal variation in gas and haze composition may be sufficient to explain the entire temperature asymmetry observed, without invoking a lag in the thermal response of the atmosphere due to dynamical inertia.

NASA Program Exobiology↗
NASA NTRS1992

Relationship of peroxyacetyl nitrate to active and total odd nitrogen at northern high latitudes: influence of reservoir species on NOx and O3

Measurements of peroxyacetyl nitrate (PAN), NO, NO2, HNO3, NOy (total odd nitrogen), and O3 were made in the high-latitude troposphere over North America and Greenland (35 degrees to 82 degrees N) during the Arctic Boundary Layer Expedition (ABLE 3A) (July-August 1988) throughout 0-to 6-km altitudes. These data are analyzed to quantitatively describe the relationships between various odd nitrogen species and assess their significance to global tropospheric chemistry. In the free troposphere, PAN was as much as 25 times more abundant than NOx. PAN to NOx ratio increased with increasing altitude and latitude. PAN was found to be the single most abundant reactive nitrogen species in the free troposphere and constituted a major fraction of NOy, PAN to NOy ratios were about 0.1 in the boundary layer and increased to 0.4 in the free troposphere. A 2-D global photochemical model with C1-C3 hydrocarbon chemistry is used to compare model predictions with measured results. A sizable portion (approximately 50%) of the gaseous reactive nitrogen budget is unaccounted for, and unknown organic nitrates and pernitrates are expected to be present. Model calculations (August 1, 70 degrees N) show that a major fraction of the observed NOx (50 to 70% of median) may find its source in the available PAN reservoir. PAN and the unknown reservoir species may have the potential to control virtually the entire NOx availability of the high latitude troposphere. It is predicted that the summer NOx and O3 mixing ratios in the Arctic/sub-Arctic troposphere would be considerably lower in the absence of the ubiquitous PAN reservoir. Conversely, this PAN reservoir may be responsible for the observed temporal increase in tropospheric O3 at high latitudes.

NASA Center ARC↗