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At least 91 records · Page 5
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NASA NTRS1991

Nighttime reactive nitrogen measurements from stratospheric infrared thermal emission observations

IR thermal emission spectra of the earth's atmosphere in the 700-2000/cm region were obtained with a cryogenically cooled high-resolution interferometer spectrometer on a balloon flight from Palestine, Texas, on September 15-16, 1986. The observations exhibit spectral features of a number of stratospheric constituents, including important species of the reactive nitrogen family. An analysis of the observed data for simultaneously measured vertical distributions of O3, H2O, N2O, NO2, N2O5, HNO3, and ClONO2 is presented. These measurements permit the first direct determination of the nighttime total reactive nitrogen concentrations, and the partitioning of the important elements of the NO(x) family. Comparisons of the total reactive nitrogen budget are made with the measurements by the ATMOS experiment and with the predictions of one-dimensional and two-dimensional photochemical models.

Abbas, Mian M.↗
NASA NTRS1990

Infrared measurements of atmospheric constituents

The objective of this program is to obtain data concerning the concentration versus altitude of various constituents of interest in the photochemistry of the stratospheric ozone layer. Data pertinent to this objective are obtained using balloon-borne instruments to measure the atmospheric transmission and emission in the mid infrared. In addition to obtaining constituent profile information, the spectral data obtained are also used to identify absorption or emission features which may interfere with the retrieval of constituent data from satellite instruments using lower spectral resolution. The spectral resolution obtained with the solar spectral system is 0.0025 cm(exp -1) and represents about a factor of 5 greater resolution than any solar spectra previously obtained in this spectral region. As a result of the increase in spectral resolution, a large number of features are observed in these spectra which were not observed in previous studies. Identification and analysis of these features is in progress. The results of this analysis to date shows a number of HNO3 features which have not been observed before, and these occur where they will interfere with the retrieval of other constituents. An example of the interference is the occurrence of features in the 780.2 cm(exp -1) region which overlap the ClONO2 feature which will be used for retrieval of ClONO2 by the CLAES instrument on UARS. A number of features due to COF2 were also identified in the 1250 cm(exp -1) region which may interfere with retrieval of N2O5.

Murcray, David G.↗
NASA NTRS1990

Stratospheric constituent distributions from balloon-based limb thermal emission measurements

This research task deals with an analysis of infrared thermal emission observations of the Earth's atmosphere for determination of trace constituent distributions. Infrared limb thermal emission spectra in the 700-2000 cm(exp -1) region were obtained with a liquid nitrogen cooled Michelson interferometer-spectrometer (SIRIS) on a balloon flight launched from Palestine, Texas, at nighttime on September 15-16, 1986. An important objective of this work is to obtain simultaneously measured vertical mixing ratio profiles of O3, H2O, N2O, NO2, N2O5, HNO3 and ClONO2 and compare with measurements made with a variety of techniques by other groups as well as with photochemical model calculations. A portion of the observed spectra obtained by SIRIS from the balloon flight on September 15-16, 1986, has been analyzed with a focus on calculation of the total nighttime odd nitrogen budget from the simultaneously measured profiles of important members of the NO(sub x) family. The measurements permit first direct determination of the nighttime total odd nitrogen concentrations NO(sub y) and the partitioning of the important elements of the NO(sub x) family.

Abbas, Mian M.↗
NASA NTRS1991

Measurements of ClO and O3 from 21 deg N to 61 deg N in the lower stratosphere during February 1988 - Implications for heterogeneous chemistry

The decline in stratospheric ozone at northern midlatitudes in wintertime may be caused by chlorine photochemistry that has been enhanced by heterogeneous reactions. The possibility that the heterogeneous reaction of N2O5 on sulfate aerosols is the cause of this decadal ozone decline is examined by comparing ClO and O3 measurements made in the lower stratosphere during February, 1988, with results from a 2D model. At midlatitudes, the abundances, latitudinal, and seasonal gradients of the observed ClO are similar to the results of a model with heterogeneous chemistry, but are in strong disagreement with the results from the model with only gas-phase chemistry. At low latitudes, agreement is best with the results of the model with only gas-phase chemistry. Limited observations indicate that the amount of reactive chlorine is being enhanced, and that heterogeneous chemistry is a likely cause.

King, J. C.↗
NASA NTRS1992

Photochemical partitioning of the reactive nitrogen and chlorine reservoirs in the high-latitude stratosphere

The correlated set of measurements in the lower stratosphere from polar missions of the NASA ER-2 is used to derive partitioning of the major components of the reactive nitrogen and inorganic chlorine reservoirs. The results provide a consistent method for comparing distributions, and hence the controlling processes, between different areas of the near-polar regions. Clear evidence of the effects of heterogeneous processes in the atmosphere is found. Values for NO2, ClONO2, N2O5, and Cl2O2 are derived in a simplified steady-state model based on in situ NO, ClO, O3, temperature, and pressure measurements, laboratory-measured reaction rates; and modeled photodissociation rates. Values for the reservoir totals are independently derived from measurements of N2O, organic chlorine, and total reactive nitrogen. The relative abundances of the measured and derived species within the reservoirs are calculated, and the longer-lived species HCl and HNO3 are estimated as the residuals of their respective reservoirs.

Kawa, S. R.↗
NASA NTRS1992

Catastrophic loss of stratospheric ozone in dense volcanic clouds

Rapid, localized loss of ozone is predicted to occur in the midlatitude and tropical stratosphere in the presence of very large concentrations of sulfate aerosols. Volcanic eruptions can increase the effective surface area of sulfuric acid so that heterogeneous reactions involving ClONO2, and secondarily N2O5, are able to suppress NO(x) abundances by more than a factor of 10 relative to gas phase chemistry. When NO(x) levels fall below a threshold, e.g., 0.6 ppb at 24 km in mid-latitudes, the chlorine-catalyzed loss of O3 proceeds at rates comparable to those during the formation of the Antarctic ozone hole, more than 50 ppb per day. If such losses occurred following the eruption of Mount Pinatubo in the most volcanically perturbed regions over the tropics and mid-latitudes, this model predicts that they are driven primarily by the suppression of NO(x) below these critical levels. The increase in stratospheric chlorine since El Chichon has made Mount Pinatubo more than twice as effective in causing rapid O3 loss.

Prather, Michael↗
NASA NTRS1992

Absorption parameters of very dense molecular spectra for the HITRAN compilation

Cross sections for the heavy molecules CFC-11, CFC-12, CFC-13, CFC-14, CFC-22, CFC-113, CFC-114, CFC-115, CCl4, ClONO2, N2O5, HNO4, and HNO3 are included on the HITRAN 91 database. For many of these species, the cross sections vary by a factor of two between room temperature and temperatures near 210 K. The chemical importance of the heavy molecules, the quantitative accuracy of the HITRAN 91 cross sections, and the need for additional spectroscopic quantification are discussed.

Massie, S. T.↗
NASA NTRS1991

An overview of the spectroscopy of the atmosphere using far infrared emission experiment (SAFIRE)

The SAFIRE experiment was conceived to satisfy a long-standing need for simultaneous middle atmosphere observations of ozone and important O(y), HO(y), NO(y), ClO(y), and BrO(y) gases, coupled with dynamics data. This will be accomplished using interferometry and broadband radiometry to sound the Earth limb in the far IR and mid IR, respectively. The experiment will employ the latest developments in detector and cryogenic cooling technology in order to achieve the measurement objectives. Detailed instrument and simulated atmospheric retrieval studies show that important gases such as OH, HO2, H2O2, HDO, N2O5, and HOCl can be observed with good accuracy.

Russell, James M., III↗
NASA NTRS1993

The cryogenic limb array etalon spectrometer (CLAES) on UARS - Experiment description and performance

The design and the performance of the cryogenic limb array spectrometer (CLAES) aboard the NASA Upper Atmosphere Research Satellite are discussed. CLAES measures altitude profiles of temperature, pressure, O3, H2O, CH4, N2O, NO, NO2, N2O5, HNO3, ClONO2, HCl, CFC 11, CFC 12, and aerosol absorption coefficients for atmospheric layer between 10 and 60 km. Examples of atmospheric spectral emission profiles for a number of constituents are presented as well as responsivity and noise parameters.

Roche, A. E.↗
NASA NTRS1993

Chemical kinetic studies of atmospheric reactions using tunable diode laser spectroscopy

IR absorption using tunable diode laser spectroscopy provides a sensitive and quantitative detection method for laboratory kinetic studies of atmospheric trace gases. Improvements in multipass cell design, real time signal processing, and computer controlled data acquisition and analysis have extended the applicability of the technique. We have developed several optical systems using off-axis resonator mirror designs which maximize path length while minimizing both the sample volume and the interference fringes inherent in conventional 'White' cells. Computerized signal processing using rapid scan (300 kHz), sweep integration with 100 percent duty cycle allows substantial noise reduction while retaining the advantages of using direct absorption for absolute absorbance measurements and simultaneous detection of multiple species. Peak heights and areas are determined by curve fitting using nonlinear least square methods. We have applied these techniques to measurements of: (1) heterogeneous uptake chemistry of atmospheric trace gases (HCl, H2O2, and N2O5) on aqueous and sulfuric acid droplets; (2) vapor pressure measurements of nitric acid and water over prototypical stratospheric aerosol (nitric acid trihydrate) surfaces; and (3) discharge flow tube kinetic studies of the HO2 radical using isotopic labeling for product channel and mechanistic analysis. Results from each of these areas demonstrate the versatility of TDL absorption spectroscopy for atmospheric chemistry applications.

Worsnop, Douglas R.↗
NASA NTRS1993

Comment on porosities of ice films used to simulate stratospheric cloud surfaces

Reference is made to a recent article by Hanson and Ravishankara (HR) containing data on the reaction probabilities of N2O5 and ClONO2 on ice films of varying thickness. In accordance with their interpretation of the observations, no correction for internal diffusion was needed and, thus, by implication, their films were effectively nonporous. Here, it is argued that vapor deposited films can be highly porous and that porous films do not always show a large increase in reactivity or uptake capacity with thickness. It is pointed out that the assumptions made by HR are responsible for the poor fit of their data.

Keyser, Leon F.↗
NASA NTRS1993

Stratospheric aircraft exhaust plume and wake chemistry

Progress to date in an ongoing study to analyze and model emissions leaving a proposed High Speed Civil Transport (HSCT) from when the exhaust gases leave the engine until they are deposited at atmospheric scales in the stratosphere is documented. A kinetic condensation model was implemented to predict heterogeneous condensation in the plume regime behind an HSCT flying in the lower stratosphere. Simulations were performed to illustrate the parametric dependence of contrail droplet growth on the exhaust condensation nuclei number density and size distribution. Model results indicate that the condensation of water vapor is strongly dependent on the number density of activated CN. Incorporation of estimates for dilution factors into a Lagrangian box model of the far-wake regime with scale-dependent diffusion indicates negligible decrease in ozone and enhancement of water concentrations of 6-13 times background, which decrease rapidly over 1-3 days. Radiative calculations indicate a net differential cooling rate of the plume about 3K/day at the beginning of the wake regime, with a total subsidence ranging between 0.4 and 1 km. Results from the Lagrangian plume model were used to estimate the effect of repeated superposition of aircraft plumes on the concentrations of water and NO(y) along a flight corridor. Results of laboratory studies of heterogeneous chemistry are also described. Kinetics of HCl, N2O5 and ClONO2 uptake on liquid sulfuric acid were measured as a function of composition and temperature. Refined measurements of the thermodynamics of nitric acid hydrates indicate that metastable dihydrate may play a role in the nucleation of more stable trihydrates PSC's.

Miake-Lye, R. C.↗
NASA NTRS1992

Modeling of the partitioning of reactive odd nitrogen in the lower stratosphere using aircraft measurements of NOy, NO, and other trace species

The objective of this research was to gain a more thorough understanding of the atmospheric processes which control the partitioning of species within the reactive nitrogen (NO(y)) reservoir in the lower stratosphere. This understanding is crucial to predicting ozone loss in the stratosphere. NO(y) is defined as NO + NO2 + HNO3 + N2O5 + ClONO2 + HO2NO2 + NO3 + particulate nitrate. The research focuses on deriving the partitioning among these species using the combined set of measurements from the NASA ER-2 aircraft during recent missions designed to study stratospheric ozone depletion.

Kawa, Stephan Randolph↗
NASA NTRS1993

Balloon-borne in situ measurements of ClO and ozone - Implications for heterogeneous chemistry and mid-latitude ozone loss

In situ measurements of chlorine oxide (ClO) obtained on 31 March 1991 with a new balloon-borne instrument are compared to results from a photochemical model which incorporates hydrolysis of N2O5 on sulfate aerosols. With the addition of this process, there is better agreement between calculation and measurement over most of the profile, except below 20 km where observed ClO is greater by as much as a factor of four. In a model which is constrained to reproduce the observed ClO below 20 km, ozone loss by catalytic cycles involving halogen oxides becomes larger than that from NO(x), which would dominate under gas-phase or standard heterogeneous conditions.

Avallone, L. M.↗
NASA NTRS1994

Effects of stratospheric aerosol surface processes on the LLNL two-dimensional zonally averaged model

We have investigated the effects of incorporating representations of heterogeneous chemical processes associated with stratospheric sulfuric acid aerosol into the LLNL two-dimensional, zonally averaged, model of the troposphere and stratosphere. Using distributions of aerosol surface area and volume density derived from SAGE II satellite observations, we were primarily interested in changes in partitioning within the Cl- and N- families in the lower stratosphere, compared to a model including only gas phase photochemical reactions. We have considered the heterogeneous hydrolysis reactions N2O5 + H2O(aerosol) yields 2 HNO3 and ClONO2 + H2O(aerosol) yields HOCl + HNO3 alone and in combination with the proposed formation of nitrosyl sulfuric acid (NSA) in the aerosol and its reaction with HCl. Inclusion of these processes produces significant changes in partitioning in the NO(y) and ClO(y) families in the middle stratosphere.

Connell, Peter S.↗
NASA NTRS1994

The chemistry of bromine in the stratosphere: Influence of a new rate constant for the reaction BrO + HO2

The impact of new laboratory data for the reaction BrO + HO2 yields HOBr + O2 in the depletion of global stratospheric ozone has been estimated using a one-dimensional photochemical model taking into account the heterogeneous reaction on sulphate aerosols which converts N2O5 into HNO3. Assuring an aerosol loading 2 times as large as the 'background' and a reaction probability of 0.1 for the above heterogeneous reaction, the 6 fold increase in the measured rate constant for the reaction of BrO with HO2 increases the computed depletion of global ozone produced by 20 ppt of total bromine from 2.01 percent to 2.36 percent. The use of the higher rate constant increases the HOBr mixing ratio and makes the bromine partitioning and the ozone depletion very sensitive to the branching ratio of the potential channel forming HBr in the BrO + HO2 reaction.

Pirre, Michel↗
NASA NTRS1994

Measurements of stratospheric constituents by ISAMS

ISAMS is a limb sounding radiometer flying on the UARS, and designed to measure temperature, pressure, O3, CO, NO, NO2, N2O5, HNO3, CH4, H2O, N2O, and aerosol. Its capabilities are described, together with the present status of validation of its data products, and plans for future improvement.

Rodgers, Clive D.↗