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NASA NTRS1994

Summertime distribution and relations of reactive odd nitrogen species and NO(y) in the troposphere over Canada

We report here large-scale features of the distribution of NO(x), HNO3, PAN, particle NO3, and NO(y) in the troposphere from 0.15 to 6 km altitude over central Canada. These measurements were conducted in July - August 1990 from the NASA Wallops Electra aircraft as part of the joint United States-Canadian Arctic Boundary Layer Expedition (ABLE) 3B-Northern Wetlands Study. Our findings show that this region is generally NO(x) limited, with NO(x) mixing ratios typically 20-30 parts per trillion by volume (pptv). We found little direct evidence for anthropogenic enhancement of mixing ratios of reactive odd nitrogen species and NO(y) above those in 'background' air. Instead, it appears that enhancements in the mixing ratios of these species were primarily due to emissions from several day old or CO-rich-NO(x)-poor smoldering local biomass-burning fires. NO(x) mixing ratios in biomass-burning impacted air masses were usually less than 50 pptv, but those of HNO3 and PAN were typically 100-300 pptv representing a twofold-threefold enhancement over 'background' air. During our study period, inputs of what appeared to be aged tropical air were a major factor influencing the distribution of reactive odd nitrogen in the midtroposphere over northeastern North America. These air masses were quite depleted in NO(y) (generally less than 150 pptv), and a frequent summertime occurrence of such air masses over this region would imply a significant influence on the reactive odd nitrogen budget. Our findings show that the chemical composition of aged air masses over subarctic Canada and those documented in the Arctic during ABLE 3A have strikingly similar chemistries, suggesting large-scale connection between the air masses influencing these regions.

Talbot, R. W.↗

NASA NTRS2007

Spectroscopic Detection of COClF in the Tropical and Mid-Latitude Lower Stratosphere

We report retrievals of COClF (carbonyl chlorofluoride) based on atmospheric chemistry experiment (ACE) solar occultation spectra recorded at tropical and mid-latitudes during 2004-2005. The COClF molecule is a temporary reservoir of both chlorine and fluorine and has not been measured previously by remote sensing. A maximum COClF mixing ratio of 99.7+/-48.0 pptv (10(exp -12) per unit volume, 1 sigma) is measured at 28km for tropical and subtropical occultations (latitudes below 20deg in both hemispheres) with lower mixing ratios at both higher and lower altitudes. Northern hemisphere mid-latitude mixing ratios (30-50degN) resulted in an average profile with a peak mixing ratio of 51.7+/-32.1 pptv, 1 sigma, at 27 km, also decreasing above and below that altitude. We compare the measured average profiles with the one reported set of in situ lower stratospheric mid-latitude measurements from 1986 and 1987, a previous two-dimensional (2-D) model calculation for 1987 and 1993, and a 2-D-model prediction for 2004. The measured average tropical profile is in close agreement with the model prediction; the northern mid-latitude profile is also consistent, although the peak in the measured profile occurs at a higher altitude (2.5-4.5km offset) than in the model prediction. Seasonal average 2-D-model predictions of the COClF stratospheric distribution for 2004 are also reported.

Rinsland, Curtis P.↗

NASA NTRS1980

Sulfate and nitrate collected by filter sampling near the tropopause

Filter samples collected near the tropopause with an F-106 aircraft and two Boeing 747 aircraft were analyzed for sulfate and nitrate ion content. Within the range of routine commercial flight altitudes (at or below 12.5 km), stratospheric mass mixing ratios for the winter-spring group averaged 0.26 ppbm for sulfate and 0.35 ppbm for nitrate. For the summer-fall group, stratosphere mixing ratios averaged 0.13 ppbm and 0.25 ppbm for sulfate and nitrate, respectively. Winter-spring group tropospheric mass mixing ratios averaged 0.08 ppbm for sulfate and 0.10 ppbm for nitrate, while summer-fall group tropospheric mixing ratios averaged 0.05 ppbm for sulfate and 0.08 ppbm for nitrate. Correlations of the filter data with available ozone data suggest that the sulfate and nitrate are transported from the stratosphere to the troposphere.

Humenik, F. M.↗

NASA NTRS2004

Analysis of the Atmospheric Distribution, Sources, and Sinks of Oxygenated Volatile Organic Chemicals Based on Measurements over the Pacific during TRACE-P

Airborne measurements of a large number of oxygenated volatile organic chemicals (OVOC) were carried out in the Pacific troposphere (0.1-12 km) in winter/spring of 2001 (24 February to 10 April). Specifically, these measurements included acetone (CH3COCH3), methylethyl ketone (CH3COC2H5, MEK), methanol (CH3OH), ethanol (C2H5OH), acetaldehyde (CH3CHO), propionaldehyde (C2H5CHO), peroxyacylnitrates (PANs) (C(sub n)H(sub 2n+1)COO2NO2), and organic nitrates (C(sub n)H(sub 2n+1)ONO2). Complementary measurements of formaldehyde (HCHO), methyl hydroperoxide (CH3OOH), and selected tracers were also available. OVOC were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Background mixing ratios were typically highest in the lower troposphere and declined toward the upper troposphere and the lowermost stratosphere. Their total abundance (Summation of OVOC) was nearly twice that of nonmethane hydrocarbons (Summation of C2-C8 NMHC). Throughout the troposphere, the OH reactivity of OVOC is comparable to that of methane and far exceeds that of NMHC. A comparison of these data with western Pacific observations collected some 7 years earlier (February-March 1994) did not reveal significant differences. Mixing ratios of OVOC were strongly correlated with each other as well as with tracers of fossil and biomass/biofuel combustion. Analysis of the relative enhancement of selected OVOC with respect to CH3Cl and CO in 12 plumes originating from fires and sampled in the free troposphere (3-11 km) is used to assess their primary and secondary emissions from biomass combustion. The composition of these plumes also indicates a large shift of reactive nitrogen into the PAN reservoir thereby limiting ozone formation. A three-dimensional global model that uses state of the art chemistry and source information is used to compare measured and simulated mixing ratios of selected OVOC. While there is reasonable agreement in many cases, measured aldehyde concentrations are significantly larger than predicted. At their observed levels, acetaldehyde mixing ratios are shown to be an important source of HCHO (and HO x ) and PAN in the troposphere. On the basis of presently known chemistry, measured mixing ratios of aldehydes and PANs are mutually incompatible. We provide rough estimates of the global sources of several OVOC and conclude that collectively these are extremely large (150-500 Tg C / yr) but remain poorly quantified.

Singh, H. B.↗

NASA NTRS2002

On the Choice of Variable for Atmospheric Moisture Analysis

The implications of using different control variables for the analysis of moisture observations in a global atmospheric data assimilation system are investigated. A moisture analysis based on either mixing ratio or specific humidity is prone to large extrapolation errors, due to the high variability in space and time of these parameters and to the difficulties in modeling their error covariances. Using the logarithm of specific humidity does not alleviate these problems, and has the further disadvantage that very dry background estimates cannot be effectively corrected by observations. Relative humidity is a better choice from a statistical point of view, because this field is spatially and temporally more coherent and error statistics are therefore easier to obtain. If, however, the analysis is designed to preserve relative humidity in the absence of moisture observations, then the analyzed specific humidity field depends entirely on analyzed temperature changes. If the model has a cool bias in the stratosphere this will lead to an unstable accumulation of excess moisture there. A pseudo-relative humidity can be defined by scaling the mixing ratio by the background saturation mixing ratio. A univariate pseudo-relative humidity analysis will preserve the specific humidity field in the absence of moisture observations. A pseudorelative humidity analysis is shown to be equivalent to a mixing ratio analysis with flow-dependent covariances. In the presence of multivariate (temperature-moisture) observations it produces analyzed relative humidity values that are nearly identical to those produced by a relative humidity analysis. Based on a time series analysis of radiosonde observed-minus-background differences it appears to be more justifiable to neglect specific humidity-temperature correlations (in a univariate pseudo-relative humidity analysis) than to neglect relative humidity-temperature correlations (in a univariate relative humidity analysis). A pseudo-relative humidity analysis is easily implemented in an existing moisture analysis system, by simply scaling observed-minus background moisture residuals prior to solving the analysis equation, and rescaling the analyzed increments afterward.

Dee, Dick P.↗

NASA NTRS1981

Gaseous constituents in the plume from eruptions of Mount St. Helens

Measurements in the stratosphere of gaseous constituents in the plume of Mount St. Helens were obtained during five flights of the NASA U-2 aircraft between 19 May and 17 June 1980. Mixing ratios from gas chromatographic measurements on samples acquired about 24 hours after the initial eruption show considerable enhancement over nonvolcanic concentrations for sulfur dioxide (more than 1000 times), methyl chloride (about 10 times), and carbon disulfide (more than 3 times). The mixing ratio of carbonyl sulfide was comparable to nonvolcanic mixing ratios although 3 days later it was enhanced two to three times. Ion chromatography measurements on water-soluble constituents are also reported. Very large concentrations of chloride, nitrate, and sulfate ions were measured, implying large mixing ratios for the water-soluble gaseous constituents from which the anions are derived. Measurements of radon-222 present in the plume are also reported.

Inn, E. C. Y.↗

NASA NTRS1994

Spring dehydration in the Antarctic stratospheric vortex observed by HALOE

The distribution of dehydrated air in the middle and lower stratosphere during the 1992 Southern Hemisphere spring is investigated using Halogen Occultation Experiment (HALOE) observations and trajectory techniques. Comparisons between previously published Version 9 and the improved Version 16 retrievals on the 700-K isentropic surface show very slight (0.05 ppmv) increases in Version 16 CH4 relative to Version 9 within the polar vortex. Version 16 H2O mixing ratios show a reduction of 0.5 ppmv relative to Version 9 within the polar night jet and a reduction of nearly 1.0 ppmv in middle latitudes when compared to Version 9. The version 16 HALOE retrievals show low mixing ratios of total hydrogen (2CH4 + H2O) within the polar vortex on both 700 and 425 K isentropic surfaces relative to typical middle-stratospheric 2CH4 + H2O mixing ratios. The low 2CH4 + H2O mixing ratios are associated with dehydration. Slight reductions in total hydrogen, relative to typical middle-stratospheric values, are found at these levels throughout the Southern Hemisphere during this period. Trajectory calculations show that middle-latitude air masses are composed of a mixture of air from within the polar night jet and air from middle latitudes. A strong kinematic barrier to large-scale exchange is found on the poleward flank of the polar night jet at 700 K. A much weaker kinematic barrier is found at 425 K. The impact of the finite tangent pathlength of the HALOE measurements is investigated using an idealized tracer distribution. This experiment suggests that HALOE should be able to resolve the kinematic barrier, if it exists.

Pierce, R. Bradley↗

NASA NTRS1983

Loss of water from Venus. I - Hydrodynamic escape of hydrogen

A one-dimensional photochemical-dynamic model is used to study hydrodynamic loss of hydrogen from a primitive, water-rich atmosphere on Venus. The escape flux is calculated as a function of the H2O mixing ratio at the atmospheric cold trap. The cold trap mixing ratio is then related in an approximate fashion to the H2O concentration in the lower atmosphere. Hydrodynamic escape should have been the dominant loss process for hydroogen when the H2O mass mixing ratio in the lower atmosphere exceeded approximately 0.1. The escape rate would have depended upon the magnitude of the solar ultraviolet flux and the atmospheric EUV heating efficiency and, to a lesser extent, on the O2 content of the atmosphere. The time required for Venus to have lost the bulk of a terrestrial ocean of water is on the order of a billion years. Deuterium would have been swept away along with hydrogen if the escape rate was high enough, but some D/H enrichment should have occurred as the escape rate slowed down.

Kasting, J. F.↗

NASA NTRS1979

Ammonia photolysis and the greenhouse effect in the primordial atmosphere of the earth

Photochemical calculations indicate that in the prebiotic atmosphere of earth ammonia would have been irreversibly converted to N2 in less than 40 years if the ammonia surface mixing ratio were no more than 0.0001. However, if a continuous outgassing of ammonia were maintained, radiative-equilibrium calculations indicate that a surface mixing ratio of ammonia of 0.0001 or greater would provide a sufficient greenhouse effect to keep the surface temperature above freezing. With a 0.0001 mixing ratio of ammonia, 60% to 70% of the present-day solar luminosity would be adequate to maintain surface temperatures above freezing. A lower limit to the time constant for accumulation of an amount of nitrogen equivalent to the present day value is 10 my if the outgassing were such as to provide a continuous surface mixing ratio of ammonia of at least 0.00001.

Kuhn, W. R.↗

NASA NTRS1988

Tropospheric nitric oxide measurements over the Amazon Basin

Horizontal and vertical distributions of nitric oxide (NO) were measured over the Amazon Basin during NASA's Global Tropospheric Experiment (GTE) Amazon Boundary Layer Experiment mission in July-August 1985. During transit flights between the Virginia coast and Manaus, Brazil, NO mixing ratios were 12-15 pptv at 5 km altitude. Values up to 200 pptv were observed in electrically active clouds. During longitudinal surveys over the Amazon region, NO mixing ratios in the lower planetary boundary layer decreased from 25-60 pptv over the central basin to 10-12 pptv in coastal regions. In the convective cloud layer or free troposphere, NO mixing ratios averaged 13 pptv in regions not influenced by biomass burning. No longitudinal trend above the mixed layer could be detected. A steep negative gradient with increasing altitude was noted within the mixed layer before midday. Mixing ratios decreased from 60 pptv at 0.2 km to about 15 pptv at the top of the mixed layer (1 km). By midday, growth of the mixed layer height and enhanced mixing reduced the gradient, and evidence for mixing of NO into the convective cloud layer was noted.

Torres, A. L.↗

NASA NTRS1994

The vertical distribution and origin of HCN in Neptune's atmosphere

Measurements and modeling of the (3-2) rotational line of hydrogen cyanide at 265.9 GHz in Neptune's atmosphere are presented. High signal-to-noise observations provide information on the HCN vertical distribution in Neptune's stratosphere. The HCN mixing ratio is found to be nearly uniform with height above the condensation level. Best fits occur for HCN distributions that have a slight increase with altitude. A least-squares analysis yields a mixing ratio of (3.2 +/- 0.8)10(exp -10) at 2 mbar and a mean mixing ratio scale height of 250(sup 750)(sub -110) km in the 0.1-3 mbar region. To interpret these results, we developed a photochemical model of HCN. HCN formation is initiated by the reaction between CH3 radicals, produced from methane photochemistry, and N atoms. The primary sink for HCN is condensation, with minor contributions from photolysis and chemical losses. Two possible sources of N atoms are investigated: (1) infall of N escaped from Triton's upper atmosphere, and (2) galactic cosmic ray (GCR) impact on internal N2. Given the uncertainties on (i) the transport and possible ionization of N in Neptune's magnetosphere, and the fate of N(+) reaching Neptune's upper atmosphere and (ii) the N2 mixing ratio in Neptune's deep atmosphere, we suggest that both sources of N atoms may significantly contibute to the formation of HCN.

Lellouch, Emmanuel↗

NASA NTRS2021

The Climatology of Carbon Monoxide on Mars as Observed by NOMAD Nadir-geometry Observations

More than a full Martian year of observations have now been made by the Nadir Occultation for MArs Discovery (NOMAD) instrument suite on-board the ExoMars Trace Gas Orbiter. Radiative transfer modeling of NOMAD observations taken in the nadir geometry enable the seasonal and global-scale variations of carbon monoxide gas in the Martian atmosphere to be characterized. These retrievals show the column-averaged volume mixing ratio of carbon monoxide to be about 800 ppmv, with significant variations at high latitudes caused by the condensation and sublimation of the background CO2 gas. Near summer solstice in each hemisphere, the CO volume mixing ratio falls to 400 ppmv in the south and 600 ppmv in the north. At low latitudes, carbon monoxide volume mixing ratio inversely follows the annual cycle of surface pressure. Comparison of our retrieved CO volume mixing ratio against that computed by the GEM-Mars general circulation model reveals a good match in their respective seasonal and spatial trends, and can provide insight into the physical processes that control the distribution of CO gas in the current Martian atmosphere.

Mars↗

NASA NTRS1990

Long-Term Trends in the Concentrations of SF6, CHClF2, and COF2 in the Lower Stratosphere from Analysis of High-Resolution Infrared Solar Occultation Spectra

Long-term trends in the concentrations of SF6, CHClF2 (CFC-22), and COF2 in the lower stratosphere have been derived from analysis of ca. 1980 and more recent infrared solar occultation spectra recorded near 32 deg N latitude at approx. 0.02/ cm resolution. Consistent sets of line parameters and spectral calibration methods have been used in the retrievals to minimize systematic error effects. Quoted error limits are 1 sigma estimated precisions. The SF6 and CHClF2 results are based on spectra recorded by balloon-borne interferometers in March 1981 and June 1988 and a comparison of these results with the Atmospheric Trace Molecule Spectroscopy (ATMOS) Experiment/Spacelab 3 measurements obtained in May 1985 near 30 deg N latitude. In the 13-18 km altitude range the mean measured SF6 mixing ratio in parts per trillion by volume (pptv) increased from 1.17 +/- 0.21 in March 1981 to 2.02 +/- 0.20 pptv in June 1988, and the CHClF2 mixing ratio below 15 km altitude increased from 51 +/- 8 pptv in March 1981 to 102 +/- 10 pptv in June 1988. The CHClF2 retrievals used new empirical CHClF2 line parameters derived from 0.03/cm resolution laboratory spectra recorded at six temperatures between 203 and 293 K; the derived mixing ratios are approx. 30% higher than obtained with earlier sets of line parameters, thereby removing a large discrepancy noted previously between IR and in situ measurements of CHClF2. Assuming an exponential growth model for fitting the trends, SF6 and CHClF2 mean increase rates of 7.4% +/- 1.9% and 9.4% +/- 1.3% /year, are obtained, respectively, which correspond to cumulative increases by factors of approx. 1.7 and -2.0 in the concentrations of these gases over the 7.2-year measurement period. Analysis of spectra recorded in October 1979 and April 1989 yields COF2 volume mixing ratios that are respectively 0.44 +/- 0.17 and 1.21 +/- 0.24 times the ATMOS/Spacelab 3 values, from which an average COF2 increase rate of 10.3 +/- 1.8%/ year over this time period has been estimated. The present results are compared with previously reported observations and trends and with one-dimensional model calculations. The model calculated trends are in reasonably good agreement with the observations.

Rinsland, C. P.↗

NASA NTRS1989

In situ observations of ClO in the Antarctic - ER-2 aircraft results from 54 deg S to 72 deg S latitude

The spatial and temporal distributions of ClO in the latitude belt from 54 to 72 deg S during the later stages of austral winter were obtained from measurements aboard the ER-2 aircraft flying at the altitude of about 18 km into the Antarctic polar vortex. Mixing ratios of about 10 parts per trillion by volume (pptv) were found in the vicinity of 55 deg S, increasing to 50 pptv at 60 deg S. A steep gradient of the ClO mixing ratio occurred in the vicinity of 65 deg S, where, at a fixed potential temperature, the value of the ClO mixing ratio increased by an order of magnitude within a very few degrees of latitude, defining the edge of the 'chemically perturbed region' (CPR). At the southern extension of the flight track, peak mixing ratios increased sharply from 800 pptv on August 23 to 1100 pptv in early September, and then increased more slowly to 1200 pptv on September 22. This corresponds to enhancements 500 times the typical mid-latitude values.

Brune, W. H.↗

NASA NTRS1985

Infrared Measurements of Atmospheric Ethane (C2H6) From Aircraft and Ground-Based Solar Absorption Spectra in the 3000/ cm Region

A number or prominent Q-branches or the upsilon(sub 7) band or C2H6 have been identified near 3000/ cm in aircraft and ground-based infrared solar absorption spectra. The aircraft spectra provide the column amount above 12 km at various altitudes. The column amount is strongly correlated with tropopause height and can be described by a constant mixing ratio of 0.46 ppbv in the upper troposphere and a mixing ratio scale height of 3.9 km above the tropopause. The, ground-based spectra yield a column of 9.0 x 10(exp 15) molecules/sq cm above 2.1 km; combining these results implies a tropospheric mixing ratio of approximately 0.63 ppbv.

Coffey, M. T.↗

NASA NTRS1985

Infrared measurements of atmospheric ethane (C2H6) from aircraft and ground-based solar absorption spectra in the 3000/cm region

A number of prominent Q-branches of the nu-7 band of C2H6 have been identified near 3000/cm in aircraft and ground-based infrared solar absorption spectra. The aircraft spectra provide the column amount above 12 km at various altitudes. The column amount is strongly correlated with tropopause height and can be described by a constant mixing ratio of 0.46 ppbv in the upper troposphere and a mixing ratio scale height of 3.9 km above the tropopause. The ground-based spectra yield a column of 9.0 x 10 to the 15th molecules/sq cm above 2.1 km; combining these results implies a tropospheric mixing ratio of approximately 0.63 ppbv.

Coffey, M. T.↗

NASA NTRS1988

Correlation of N2O and ozone in the Southern Polar vortex during the airborne Antarctic ozone experiment

In situ N20 mixing ratios, measured by an airborne laser spectrometer (ATLAS), have been used along with in situ ozone measurements to determine the correlation of N2O and ozone in the Antarctic stratosphere during the late austral winter. During the 1987 Airborne Antarctic Ozone Experiment (AAOE), N2O data were collected by a laser absorption spectrometer on board the ER-2 on five ferry flights between Ames Research Center (37 deg N) and Punta Arenas, Chile (53 deg S), and on twelve flights over Antarctica (53 S to 72 S). Of all the trace gas species measured by instruments on board the ER-2, only one showed a relationship to the N2O/O3 correlations in the vortex. With few exceptions, positive N20/O3 correlations coincided with total water mixing ratios of greater than 2.9 ppmv, and total water mixing ratios of less than 2.9 ppmv corresponded to negative correlations. The lower water mixing ratios, or dehydrated regions, are colocated with the negative correlations within the vortex, while the wetter regions always occur near the vortex edge.

Strahan, S. E.↗

NASA NTRS2003

Chemical and Physical Properties of Bulk Aerosols within Four Sectors Observed during TRACE-P

Chemical and physical aerosol data collected on the DC-8 during TRACE-P were grouped into four sectors based on back trajectories. The four sectors represent long-range transport from the west (WSW), regional circulation over the western Pacific and Southeast Asia (SE Asia), polluted transport from Northern Asia with substantial sea salt at low altitudes (NNW) and a substantial amount of dust (Channel). WSW has generally low mixing ratios at both middle and high altitudes, with the bulk of the aerosol mass due to non-sea-salt water-soluble inorganic species. Low altitude SE Asia also has low mean mixing ratios in general, with the majority of the aerosol mass comprised of non-sea-salts, however, soot is also relatively important m this region. "w had the highest mean sea salt mixing ratios, with the aerosol mass at low altitudes (a km) evenly divided between sea salts, mm-sea-salts, and dust. The highest mean mixing ratios of water-soluble ions and soot were observed at the lowest altitudes (a km) in the Channel sector. The bulk of the aerosol mass exported from Asia emanates h m Channel at both low and midaltitudes, due to the prevalence of dust compared to other sectors. Number densities show enhanced fine particles for Channel and NNW, while their volume distributions are enhanced due to sea salt and dust Low-altitude Channel exhibits the highest condensation nuclei ((34) number densities along with enhanced scattering coefficients, compared to the other sectors. At midaltitudes (2-7 km), low mean CN number densities coupled with a high proportion of nonvolatile particles (265%) observed in polluted sectors (Channel and NNW) are attributed to wet scavenging which removes hygroscopic CN particles. Low single scatter albedo m SE Asia reflects enhanced soot

Jordan, C. E.↗