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NASA NTRS1994

Reevaluation of the NOAA/CMDL carbon monoxide reference scale and comparisons with CO reference gases at NASA-Langley and the Fraunhofer Institut

The carbon monoxide (CO) reference scale created by the National Oceanic and Atmospheric Administration/Climate Monitoring and Diagnostics Laboratory (NOAA/CMDL) is used to quantify measurements of CO in the atmosphere, calibrate standards of other laboratories and to otherwise provide reference gases to the community measuring atmospheric CO. This reference scale was created based upon a set of primary standards prepared by gravimetric methods at CMDL and has been propagated to a set of working standards. In this paper we compare CO mixing ratios assigned to the working standards by three approaches: (1) calibration against the original gravimetric standards, (2) calibration using only working standards as the reference gas, and (3) calibration against three new gravimetric standards prepared to CMDL. The agreement between these values was typically better than 1%. The calibration histories of CMDL working standards are reviewed with respect to expected rates of CO change in the atmosphere. Using a Monte Carlo approach to simulate the effect of drifting standards on calculated mixing ratios, we conclude that the error solely associated with the maintenance of standards will limit the ability to detect small CO changes in the atmosphere. We also report results of intercalibration experiments conducted between CMDL and the Diode Laser Sensor Group (DACOM) at the NASA Langley Research Center (Hampton, Virginia), and CMDL and the Fraunhofer-Institut (Garmisch-Partenkirchen, Germany). Each laboratory calibrated several working standards for CO using their reference gases, and these results were compared to calibrations conducted by CMDL. The intercomparison of eight standards (CO concentrations between approximately 100 and approximately 165 ppb) by CMDL and NASA agreed to better than +/- 2%. The calibration of six standards (CO concentrations between approximately 50 and approximately 210 ppb) by CMDL and the Fraunhofer-Institut agreed to within +/- 2% for four standards, and to within +/- 5% for all six standards.

Novelli, P. C.↗

NASA NTRS1985

High atmospheric NO(x) levels and multiple photochemical steady states

The rate of removal of atmospheric NO(x) compounds at different NO(x) levels is estimated using a one-dimensional photochemical model. NO(x) removal by wet deposition, surface deposition, and thermochemical processes is examined. NO(x) removal rates at different surface NO mixing ratios are calculated and the data are analyzed. It is revealed that at low NO(x) levels NO(x) is photochemically converted to HNO3 by either wet or dry deposition; however, at high NO(x) levels formation of HNO3 is inhibited due to the disappearance of tropospheric ozone and OH, and the NO(x) is removed by rainout of N2O4 and N2O5, surface deposition of NO and NO2, and direct dissolution of NO and NO2 in rainwater. The effects of NO(x) mixing ratios greater than 10 to the -7th on the ozone and climate are investigated.

Kasting, J. F.↗

NASA NTRS1991

In situ measurements of midlatitude ClO in winter

In situ measurements of ClO in the winter lower stratosphere are presented for six flights of the NASA ER-2 aircraft from 38 deg N to 61 deg N. Enhanced abundances, increasing in severity with date, were observed below 20 km, where HCl and ClONO2 dominate the inorganic chlorine budget. The greatest mixing ratios, over 150 pptv, were encountered on February 20 and 21, 1989, as the vortex experienced a major warming. Although the timing of these ClO enhancements and the evidence that vortex air can reach midlatitudes suggest that heterogeneous conversion of chlorine compounds within the vortex influences chemistry at midlatitudes, the enhacements observed early in the winter could have been caused by unknown chemistry occurring outside the vortex. In either case, photochemical loss of ozone due to catalytic reactions involving ClO at these mixing ratios may be responsible in part for the ozone decreases observed at high latitudes in the Northern Hemisphere.

Toohey, D. W.↗

NASA NTRS1998

Contrast Between 1992 and 1997 High Latitude Spring Haloe Observations of Lower Stratospheric HCl

HCl measurements from HALOE in the northern hemisphere during mid-May 1997 revealed vortex fragments in which the chlorine reservoir partitioning was strongly pushed toward HCl (approx. 90% HCl, approx. 10% ClONO2), similar to partitioning previously observed in the Antarctic vortex region. In contrast, observations of ClONO2 and HCl in the northern polar spring, 1992, and in other years, show these species established the balance typical for gas phase photochemical reactions in this region (approx. 60% HCl, approx. 40% ClONO2). Annually, chlorine reservoirs in the winter lower stratosphere polar vortex are converted to chlorine radicals via heterogeneous reactions on particle surfaces at very cold temperatures (less than about 200 K). As temperatures warm in spring, the heterogeneous processes become insignificant compared with gas phase reactions, and the chlorine reservoirs are reformed. Measurements through the northern winter/spring in 1992 show rapid formation of ClONO2, followed by steady loss of ClONO2 and increasing HCl. Although ClONO2 measurements are not available for 1997, the HCl increase in 1997 is observed to be much more rapid and the eventual HCl mixing ratio is about 50% greater than that of 1992. The observations are examined through comparison with the Goddard three-dimensional chemistry and transport model. This model utilizes winds and temperatures from the Goddard Earth Observing System Data Assimilation System and a complete integration scheme for stratospheric photochemistry. Analysis of the evolution of HCl and ClONO2 shows that the observed difference in the overall rate of HCl formation is explained by the sensitivity of the gas-phase chemistry to the ozone mixing ratio and the temperature. The results show that the model accurately simulates HCl and ClONO2 evolution during these two winters. Model validity is further supported by comparisons with O3 and reactive nitrogen species NO and NO2. This analysis provides a sensitive test of the lower stratospheric chlorine photochemistry, particularly because the analysis considers constituent evolution at a time when the HCl and ClONO2 are far from a photochemical stationary state.

Douglass, A. R.↗

NASA NTRS1987

The spectra of Uranus and Neptune at 8-14 and 17-23 microns

The 3-m NASA Infrared Telescope Facility was used to observe the disks of Uranus and Neptune between May 30 and June 1, 1985 in the 7-14 and 17-23 micron spectral regions. Maximum stratospheric mixing ratios of 9 x 10 to the -9th for C2H2, and of 2 x 10 to the -8th for C2H6, are found for Uranus, and the spectrum is otherwise smooth, consistent with the opacity provided by H2 collision-induced absorption and spectrally continuous stratospheric emission. Strong emission features of CH4 and C2H6 are found in the short-wavelength spectrum of Neptune, and the spectrum near 13.5 microns is consistent with C2H2 emission in local saturation equilibrium with a maximum mixing ratio of 9 x 10 to the -7th.

Orton, Glenn S.↗

NASA NTRS2005

Lidar Applications in Atmospheric Dynamics: Measurements of Wind, Moisture and Boundary Layer Evolution

A large array of state-of-the-art ground-based and airborne remote and in-situ sensors were deployed during the International H2O Project (THOP), a field experiment that took place over the Southern Great Plains (SGP) of the United States from 13 May to 30 June 2002. These instruments provided extensive measurements of water vapor mixing ratio in order to better understand the influence of its variability on convection and on the skill of quantitative precipitation prediction (Weckwerth et all, 2004). Among the instrument deployed were ground based lidars from NASA/GSFC that included the Scanning Raman Lidar (SRL), the Goddard Laboratory for Observing Winds (GLOW), and the Holographic Airborne Rotating Lidar Instrument Experiment (HARLIE). A brief description of the three lidars is given below. This study presents ground-based measurements of wind, boundary layer structure and water vapor mixing ratio measurements observed by three co-located lidars during MOP at the MOP ground profiling site in the Oklahoma Panhandle (hereafter referred as Homestead). This presentation will focus on the evolution and variability of moisture and wind in the boundary layer when frontal and/or convergence boundaries (e.g. bores, dry lines, thunderstorm outflows etc) were observed.

Demoz, Belay↗

NASA NTRS1995

Aerosol effects and corrections in the Halogen Occultation Experiment

The eruptions of Mt. Pinatubo in June 1991 increased stratospheric aerosol loading by a factor of 30, affecting chemistry, radiative transfer, and remote measurements of the stratosphere. The Halogen Occultation Experiment (HALOE) instrument on board Upper Atmosphere Research Satellite (UARS) makes measurements globally for inferring profiles of NO2, H2O, O3, HF, HCl, CH4, NO, and temperature in addition to aerosol extinction at five wavelengths. Understanding and removing the aerosol extinction is essential for obtaining accurate retrievals from the radiometer channels of NO2, H2O and O3 in the lower stratosphere since these measurements are severely affected by contaminant aerosol absorption. If ignored, aerosol absorption in the radiometer measurements is interpreted as additional absorption by the target gas, resulting in anomalously large mixing ratios. To correct the radiometer measurements for aerosol effects, a retrieved aerosol extinction profile is extrapolated to the radiometer wavelengths and then included as continuum attenuation. The sensitivity of the extrapolation to size distribution and composition is small for certain wavelength combinations, reducing the correction uncertainty. The aerosol corrections extend the usable range of profiles retrieved from the radiometer channels to the tropopause with results that agree well with correlative measurements. In situations of heavy aerosol loading, errors due to aerosol in the retrieved mixing ratios are reduced to values of about 15, 25, and 60% in H2O, O3, and NO2, respectively, levels that are much less than the correction magnitude.

Hervig, Mark E.↗

NASA NTRS1993

Stratospheric N2O5, CH4, and N2O Profiles from IR Solar Occultation Spectra

Stratospheric volume mixing ratio profiles of N2O5, CH4, and N2O have been retrieved from a set of 0.052/ cm resolution (FWHM) solar occultation spectra recorded at sunrise during a balloon flight from Aire sur I'Adour, France (44 deg N latitude) on 12 October 1990. The N2O5 results have been derived from measurements of the integrated absorption by the 1246/ cm band. Assuming a total intensity of 4.32 x 10(exp 17)cm(exp -1) molecule sq cm(exp -2) independent of temperature, the retrieved N2O5 volume mixing ratios in ppbv (parts per billion by volume, 10(exp -9)), interpolated to 2 km height spacings, are 1.64 +/- 0.49 at 37.5 km, 1.92 +/- 0.56 at 35.5 km, 2.06 +/- 0.47 at 33.5 km, 1.95 +/- 0.42 at 31.5 km, 1.60 +/- 0.33 at 29.5 km, 1.26 +/- 0.28 at 27.5 km, and 0.85 +/- 0.20 at 25.5 km. Error bars indicate the estimated I-sigma uncertainty including the error in the total band intensity (+/- 20% has been assumed). The retrieved profiles are compared with previous measurements and photochemical model results.

Peyeret, C. Camy↗

NASA NTRS2002

Raman Lidar Profiling of Aerosols Over the Central US; Diurnal Variability and Comparisons with the GOCART Model

We use profiles of aerosol extinction, water vapor mixing ratio, and relative humidity measured by the ARM SGP Raman lidar in northern Oklahoma to show how the vertical distributions of aerosol extinction and water vapor vary throughout the diurnal cycle. While significant (20-30%) variations in aerosol extinction occurred near the surface as well as aloft, smaller (approximately 10%) variations were observed in the diurnal variability of aerosol optical thickness (AOT). The diurnal variations in aerosol extinction profiles are well correlated with corresponding variations in the average relative humidity profiles. The water vapor mixing ratio profiles and integrated water vapor amounts generally show less diurnal variability. The Raman lidar profiles are also used to evaluate the aerosol optical thickness and aerosol extinction profiles simulated by the GOCART global aerosol model. Initial comparisons show that the AOT simulated by GOCART was in closer agreement with the AOT derived from the Raman lidar and Sun photometer measurements during November 2000 than during September 2000. For both months, the vertical variability in average aerosol extinction profiles simulated by GOCART is less than the variability in the corresponding Raman lidar profiles.

Ferrare, R. A.↗

NASA NTRS2011

Quantifying Spatial and Seasonal Variability in Atmospheric Ammonia with In Situ and Space-Based Observations

Ammonia plays an important role in many biogeochemical processes, yet atmospheric mixing ratios are not well known. Recently, methods have been developed for retrieving NH3 from space-based observations, but they have not been compared to in situ measurements. We have conducted a field campaign combining co-located surface measurements and satellite special observations from the Tropospheric Emission Spectrometer (TES). Our study includes 25 surface monitoring sites spanning 350 km across eastern North Carolina, a region with large seasonal and spatial variability in NH3. From the TES spectra, we retrieve a NH3 representative volume mixing ratio (RVMR), and we restrict our analysis to times when the region of the atmosphere observed by TES is representative of the surface measurement. We find that the TES NH3 RVMR qualitatively captures the seasonal and spatial variability found in eastern North Carolina. Both surface measurements and TES NH3 show a strong correspondence with the number of livestock facilities within 10 km of the observation. Furthermore, we find that TES H3 RVMR captures the month-to-month variability present in the surface observations. The high correspondence with in situ measurements and vast spatial coverage make TES NH3 RVMR a valuable tool for understanding regional and global NH3 fluxes.

Pinder, Robert W.↗

NASA NTRS2015

Comparison of Surface and Column Variations of CO2 Over Urban Areas for Future Active Remote CO2 Sensors

High resolution in-situ CO2 measurements were recorded onboard the NASA P-3B during the DISCOVER-AQ (Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality) Field Campaign, to investigate the ability of space-based observations to accurately assess near surface conditions related to air quality. This campaign includes, Washington DC/Baltimore, MD (July 2011), San Joaquin Valley, CA (January - February 2013), Houston, TX (September 2013), and Denver, CO (July-August 2014). Each of these campaigns consisted of missed approaches and approximately two hundred vertical soundings of CO2 within the lower troposphere (surface to about 5 km). In this study, surface (0 - 1 km) and column-averaged (0 - 3.5 km) CO2 mixing ratio values from the vertical soundings in the four geographically different urban areas are used to investigate the temporal and spatial variability of CO2 within the different urban atmospheric emission environments. Tracers such as CO, CH2O, NOx, and NMHCs are used to identify the source of CO2 variations in the urban sites. Additionally, we apply nominal CO2 column weighting functions for potential future active remote CO2 sensors operating in the 1.57-microns and 2.05-microns measurement regions to convert the in situ CO2 vertical mixing ratio profiles to variations in CO2 column optical depths, which is what the active remote sensors actually measure. Using statistics calculated from the optical depths at each urban site measured during the DISCOVER-AQ field campaign and for each nominal weighting function, we investigate the natural variability of CO2 columns in the lower troposphere; relate the CO2 column variability to the urban surface emissions; and show the measurement requirements for the future ASCENDS (Active Sensing of CO2 Emissions over Nights, Days, and Seasons) in the continental U.S. urban areas.

Choi, Yonghoon↗

NASA NTRS1986

Neutral oxygen and sulfur densities in the Io torus

Ultraviolet spectra (1150-1750 A) of the Io torus, obtained using a rocket-borne telescope and spectrometer in May 1981, show emissions of neutral sulfur and neutral oxygen, as well as ionic emissions of S II, S III, and S IV. The emissions are observed almost 180 deg from the location of the satellite Io and imply the existence of an extended neutral atomic cloud associated with the torus. In the present work, neutral densities and ion mixing ratios are derived by modeling the observations using torus electron temperature and density profiles proportional to those at the time of the Voyager 1 encounter. The model includes the effects of photoexcitation, which can be considerable if the neutral cloud is large enough. At the time of the observation, substantial densities of neutral oxygen and neutral sulfur are found in regions of the torus far from Io. These lower limits on the neutral densities are compared to theoretical models of the neutral source, and the ion mixing ratios are compared to IUE observations of the torus obtained over a period of 5 yr. Arguments that tend to rule out Europa as the source of the neutral emission are also presented.

Skinner, T. E.↗

NASA NTRS2021

Testing Short-term Variability and Sampling of Primary Volatiles in Comet 46P/Wirtanen

The exceptionally favorable close approach of Jupiter-family comet 46P/Wirtanen in 2018 December enabled characterization of its primary volatile composition with exceptionally high spatial resolution and sensitivities using the iSHELL spectrograph at the NASA Infrared Telescope Facility on Maunakea, HI. We sampled emissions from H2O, HCN, C2H2, NH3,C2H6, and CH3OH on UT 2018 December 21 using two instrumental settings that spanned the 2.9–3.6μm spectral region. We also obtained a sensitive 3σupper limit for H2CO and for the rarely studied molecule HC3N. We report rotational temperatures, production rates, and mixing ratios(relative to H2O as well as to C2H6). We place our results in context by comparing them with other comets observed at near-IR wavelengths. We also compare our results with those obtained using the NIRSPEC-2 spectrograph on Keck II on UT December 17 and 18 and with results obtained from iSHELL on other dates during the same apparition. Within1–2σ uncertainty, production rates obtained for all molecules in this work were consistent with those obtained using NIRSPEC-2 except H2O, indicating low-level variability on a timescale of days. Mixing ratios with respect to H2O in 46P/Wirtanen were consistent with corresponding values from NIRSPEC-2 within the uncertainty with the exception of CH3OH, which yielded a higher ratio on December 21. Our measurements afforded a high temporal resolution that spanned∼2/3 of the rotational period of 46P/Wirtanen, enabling us to test short-term variability in the production rates of H2O and HCN due to rotational effects. Both H2O and HCN production rates showed similar temporal variability, resulting in nearly constant HCN/H2O

Younas Khan↗

NASA NTRS1994

Long term trend of selected halogenated hydrocarbons

The so-called 'Library of Background Air' at the Oregon Graduate Institute was used to determine the trend in volume mixing ratios of selected halogenated hydrocarbons in the time period 1977-1989. This library consists of background air samples most of them taken at Cape Meares (Oregon). For storage stainless steel containers are used. Tests have shown the gases under consideration to be stable in these containers. Analyses using a GC/MS-system were performed for the CFCs 11, 12, 12B1 (HALON 1211, CBrClF2), 22, 113, 114 and CH3Cl, CH3Br, CH3CCl3, CCl4. The advantage of this unique investigation: different aged air samples are analyzed at the same time with the same instrument. No calibrations or intercalibrations are needed. All data are presented in normalized mixing ratios versus time. We discuss the results, derive rate constants and present a formula to describe the nonlinear increases.

Borchers, R.↗

NASA NTRS1977

Gradients of meteorological parameters in convective and nonconvective areas

Horizontal gradients of geopotential height, temperature, and wind speed were computed at the 850-, 700-, 500-, and 200-mb levels. Mixing ratio gradients also were computed, but only for the 850-, 700-, and 500-mb levels. Rawinsonde data was provided at 3- to 6-h intervals. Cumulative frequency distributions and statistical parameters showed that the variability and magnitude of the gradients decreased as the gradients were computed over progressively longer distances. Most frequency distributions were positively skewed, and the standard deviations of the gradient distributions were roughly half as large as the means. An examination of the differences of gradients observed in convective and nonconvective areas was made after convective areas were determined objectively using Manually Digitized Radar data. The gradients of height, wind speed, and mixing ratio at 850 mb were larger in convective than nonconvective areas. No general relationship held for the meteorological variables at other levels. Intensive examination of the gradients observed near squall lines revealed typical gradient patterns and trends in the magnitudes of the gradients associated with convective systems.

Mccown, M. S.↗

NASA NTRS1980

Upper atmosphere modifications due to chronic discharges of water vapor from space launch vehicle exhausts

The influences of transport, photodissociation, and frequency of injection on the global redistribution of water deposited in the earth's upper atmosphere by repeated launches of large rockets are investigated. Measurable environmental effects of the injected water are found to occur when the mesospheric water vapor mixing ratio exceeds 100 ppmv, which occurs over areas of order 20,000 sq km in connection with possible future Satellite Power System activities. These effects include (1) a 50% reduction in D-region ionization due to screening of L alpha radiation by water; (2) a 50% reduction of D-region ionization as a result of converting NO(+) to water cluster ions which possess more rapid recombination rates; (3) a doubling of OH concentrations below 100 km; and (4) a global doubling of nighttime E-region ionization due to L alpha and L beta radiations geocoronally scattered by atomic hydrogen released by photolysis of H2O. Mixing ratios of 1,000 ppmv necessary for the maintenance of clouds at the mesopause are reached only over areas of order 200 sq km.

Forbes, J. M.↗

NASA NTRS1997

Upper Tropospheric/Lower Stratospheric Distribution of Reactive Nitrogen and Ozone

In-situ measurements of a large number of trace chemicals from upper troposphere/lower stratosphere (UT/LS) were performed with the NASA DC-8 aircraft during February/March 1994 over the Pacific Ocean (10 S to 60 N). Mixing ratios in the UT were relatively low in the warm tropical and subtropical air south of the polar jetstream (approx. =28 N) but increased sharply with latitude in the cold polar air north of the jetstream. At about 45 N, high concentrations of PAN (300 ppt) coexisted with extremely low (approx. = 20 ppt) concentrations of NOx. Elevated NOx levels in the UT did not always correspond to continental outflow conditions. Deepest penetrations into the stratosphere (550 ppb O3, 279 ppb NOx, and 350 K potential temperature) corresponded to a region that has been defined as the 'lowermost stratosphere' (LS) by Holton et al. Analysis of data shows that the mixing ratios of long-lived tracer species (e.g., CH4, HNO3, NOy, CFCs, HCFCs) are linearly correlated with those of O3 and N2O. A delta-NOY/delta-O3 of 0.0054 ppb/ppb and delta-NOy/delta-N2O of -0.081 ppb/ppb is in good agreement with other reported measurements from the DC-8. These slopes are however, somewhat steeper than those reported from the ER-2 studies. We find that the reactive nitrogen budget in the UT/LS is largely balanced with shortfalls that are no greater than 15%. A number of oxygenated species (e.g., acetone, H2O2) are present and may provide an important in-situ source of HOx in the UT/LS region.

Singh, H. S.↗

NASA NTRS2002

Enhanced ClO from 10 to 12 km Near the Winter Polar Tropopause During SOLVE/THESEO-2000

Abundances of chlorine oxide have been measured in situ near the tropopause from the NASA DC-8 aircraft during the SOLVE/THESEO-2000 campaign. Significant abundances, averaging 15-20 parts per trillion, were observed throughout the lowermost stratosphere at high latitudes during winter. Mixing ratios of ClO generally increased with increasing ozone (the latter an indicator of stratospheric air) as has been observed at other latitudes and seasons. However, the ratio of ClO to inorganic chlorine ([ClO]/[Cl(sub y)]) was found to be largest in air characterized by low abundances of ozone (approximately l00-250). It was within this range of ozone values that cirrus clouds were also observed occasionally throughout the measurement period, although distinct enhancements of ClO were not commonly observed directly within cirrus clouds. Elevated abundances of ClO were also apparently observed in polar darkness. However, we attribute these measurements to OClO, a species that can also be detected by the DC-8 instrument under the conditions encountered during SOLVE/THESEO-2000. Using a photochemical box model constrained by daytime abundances of ClO, we infer that BrO mixing ratios in this region were approximately 2-4 ppt, consistent with previous measurements from balloon-borne remote sensors.

Toohey, Darin W.↗