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All sourcesNASA NTRSDOE OSTI
NASA NTRS1988

Heterogeneous chemistry related to Antarctic ozone depletion: Reaction of ClONO2 and N2O5 on ice surfaces

Laboratory studies of heterogeneous reactions of possible importance for Antarctic ozone depletion were performed. In particular, the reactions of chlorine nitrate (ClONO2) and dinitrogen pentoxide (N2O5) were investigated on ice and HCl/ice surfaces. These reactions occur on the surfaces of polar stratospheric clouds (PSCs) over Antarctica. One reaction transforms the stable chlorine reservoir species (ClONO2 and HCl) into photochemically active chlorine in the form of HOCl and Cl2. Condensation of HNO3 in the reactions removes odd nitrogen from the stratosphere, a requirement in nearly all models of Antarctic ozone depletion. Other reactions may also be important for Antarctic ozone depletion. Like the reactions of chlorine nitrate, these reactions deplete odd nitrogen through HNO3 condensation. In addition, one reaction converts a stable chlorine reservior species (HCl) into photochemically active chlorine (ClNO2). These reactions were studied with a modified version of a Knudsen cell flow reactor.

Tolbert, Margaret A.↗
NASA NTRS1988

Mass accommodation coefficient measurements for HNO3, HCl and N2O5 on water, ice and aqueous sulfuric acid droplet surfaces

Preliminary results are reported of the direct measurement of accommodation coefficients for HNO3, N2O5 and HCl on water drops, aqueous sulfuric acid drops and ice particles. The heterogeneous chemistry of these species together with ClONO2 has been implicated in the ozone depletion observed in the Antarctic stratosphere during the spring in the last eight years. The most plausible chemical mechanism involves the removal of nitrogen oxide species via condensation on ice particles in polar stratospheric clouds resulting in a increase in the active chlorine species responsible for the ozone depletion. The observation of low NO2 and high ClO densities in the Antarctic stratosphere last summer appear to be consistent with such a mechanism.

Worsnop, Douglas↗
NASA NTRS1988

Measurement of nighttime stratospheric N2O5 from infrared emission spectra

The mixing ratio profile of N2O5 has been inferred from high-resolution emission spectra obtained with a balloon-borne Fourier spectrometer. The observations were taken for the period from midnight to predawn on September 16, 1986 at 32 deg N latitude. The inferred volume mixing ratio from nighttime average spectra has a peak of about 1.8 x 10 to the -9th in the 32-35 altitude range. The inferred mixing ratio is generally less than the theoretical predictions from a one-dimensional model.

Kunde, V. G.↗
NASA NTRS1988

High resolution, balloon-borne emission spectroscopy of trace species in the lower stratosphere - N2O5, HNO3

A liquid-nitrogen cooled Fourier transform spectrometer (SIRIS) measures thermal limb-emission of the stratosphere from a balloon platform at a nominal altitude of 40 km, under night and day conditions, with a 3 km vertical resolution. N2O5 and HNO3 mixing ratios inferred from emission spectra are compared with previous measurements and with the predictions from a one-dimensional photochemical model.

Brasunas, J.↗
NASA NTRS1994

Measurements of stratospheric NO, NO2, and N2O5 by ISAMS: Preliminary observations and data validation

The Improved Stratospheric and Mesospheric Sounder (ISAMS) is a multichannel radiometer and forms part of the science payload of the Upper Atmosphere Research Satellite (UARS). ISAMS measures infrared emissions from the Earth's atmosphere in several wavelength bands. Three such bands include emission from nitric oxide, nitrogen dioxide, and dinitrogen pentoxide. In this paper, we briefly discuss how the ISAMS instrument measures NO, NO2, and N2O5. We also present preliminary data from these channels and describe preliminary validation work.

Kerridge, Brian J.↗
NASA NTRS1994

Balloon profiles of stratospheric NO2 and HNO3 for testing the heterogeneous hydrolysis of N2O5 on sulfate aerosols

Simultaneous in situ measurements of stratospheric NO2, HNO3, HCl, and CH4 from 34 to 24 km were made in August 1992 from Palestine, Texas, using the Balloon-borne Laser In-Situ Sensor (BLISS) tunable diode laser spectrometer. Although the measurements of NO2, HNO3, and NO2/HNO3 agree well with gas-phase model calculations near 34 km where Stratospheric Aerosol and Gas Experiment (SAGE) 2 data show little sulfate aerosol, this is not true at the lower altitudes where SAGE 2 shows high aerosol loadings. At 24 km the BLISS NO2 and HNO3 measurements are 70% lower and 50% higher, respectively, than the gas phase model predictions, with a measured NO2/HNO3 ratio 5 times smaller. When the heterogeneous hydrolysis of N2O5 and ClONO2 on sulfate aerosol of surface area densities matching the SAGE 2 measurements is added to the model, good agreement with the BLISS measurements is found over the whole altitude range.

Webster, C. R.↗
NASA NTRS1994

The reaction probability of N2O5 with sulfuric acid aerosols at stratospheric temperatures and compositions

We have measured the rate of reaction of N2O5 with H2O on monodisperse, submicrometer H2SO4 particles in a low-temperature flow reactor. Measurements were carried out at temperatures between 225 K and 293 K on aerosol particles with sizes and compositions comparable to those found in the stratosphere. At 273 K, the reaction probability was found to be 0.103 +/- 0.0006, independent of H2SO4 composition from 64 to 81 wt%. At 230 K, the reaction probability increased from 0.077 for compositions near 60% H2SO4 to 0.146 for compositions near 70% H2SO4. Intermediate conditions gave intermediate results except for low reaction probabilities of about 0.045 at 260 K on aerosols with about 78% H2SO4. The reaction probability did not depend on particle size. These results imply that the reaction occurs essentially at the surface of the particle. A simple model for this type of reaction that reproduces the general trends observed is presented. the presence of formaldehyde did not affect the reaction rate.

Fried, Alan↗
NASA NTRS1995

Heterogeneous Reactions of HNO3(g) + NaCl(s) Yields HCL(g) + NaNO3(s) and N2O5(g) + NaCl(s) Yields ClNo2(g) + NaNO3(s)

The heterogeneous reactions of HNO3(g) + NaCl(s) Yields HCL(g) + NaNO3(s) and N2O5(g) + NaCl(s) Yields ClNo2(g) + NaNO3(s)were investigated over a temperature range of 223-296 K in a flow-tube reactor coupled to a quadrupole mass spectrometer. The implications for volcanic enhancement of the HCl and HNO3 column density in the lower stratosphere are discussed.

heterogeneous↗
NASA NTRS1990

Stratospheric NO, NO2, and N2O5 - A comparison of model results with Spacelab 3 Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements

The Spacelab 3 Atmospheric Trace Molecule Spectroscopy measurements in 1985 of stratospheric NO/NO2 abundance ratios were compared with abundance ratios calculated using a time-dependent photochemical model. A good agreement between calculated and observed values of the NO/NO2 abundance ratio was found through much of the stratosphere, indicating that the temperature-dependent rate constant K3 (NO + O3) used in the model is properly parameterized.

Allen, Mark↗
NASA NTRS1992

Heterogeneous conversion of N2O5 to HNO3 on background stratospheric aerosols - Comparisons of model results with data

The effects of heterogeneous processing by a parameterized lower stratospheric sulfate aerosol layer on model calculations were examined using a 2D photochemical model. Model results were compared with zonally averaged LIMS data on HNO3 and NO2 and in situ measurements of NO, NO(y), and ClO, taken by the ER-2 aircraft. The results obtained are contradictory: some comparisons favor heterogeneous chemistry, and some do not. It is suggested that the assumptions made to parameterize the sulfate aerosol chemistry result in a rate of heterogeneous processing that is too vigorous.

Considine, David B.↗
NASA NTRS1991

Stratospheric photochemical studies with Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements

The photochemical partitioning of stratospheric odd chlorine and odd nitrogen is examined utilizing diurnal model calculations and data from the ATMOS experiment. This experiment, conducted during April-May 1985, employed a solar occultation method to obtain vertical profiles of temperature and various other trace constituents at 30 deg N and 48 deg S latitudes. The ATMOS data set confirms the presence of N2O5 in the stratosphere; however, the observed mixing ratios at sunset are more than a factor of 2 less than the calculated values. It is shown that the conversion of N2O5 into HNO3 could take place in the presence of aerosol surfaces quickly enough to affect the N2O5 mixing ratio below 30 km. Inclusion of the heterogeneous reaction brings the calculated N2O5 profile below 30 km into closer agreement with the ATMOS data.

Natarajan, Murali↗
NASA NTRS1990

Thermal emission spectroscopy of the middle atmosphere

The general objective of this research is to obtain, via remote sensing, simultaneous measurements of the vertical distributions of stratospheric temperature, ozone, and trace constituents that participate in the catalytic destruction of ozone (NO(sub y): NO, NO2, NO3, HNO3, ClONO2, N2O5, HNO4; Cl(sub x): HOCl), and the source gases for the catalytic cycles (H2O, CH4, N2O, CF2Cl2, CFCl3, CCl4, CH3Cl, CHF2Cl, etc.). Data are collected during a complete diurnal cycle in order to test our present understanding of ozone chemistry and its associate catalytic cycles. The instrumentation employed is an emission-mode, balloon-borne, liquid-nitrogen-cooled Michelson interferometer-spectrometer (SIRIS), covering the mid-infrared range with a spectral resolution of 0.020 cm(exp -1). Cryogenic cooling combined with the use of extrinsic silicon photoconductor detectors allows the detection of weak emission features of stratospheric gaseous species. Vertical distributions of these species are inferred from scans of the thermal emission of the limb in a sequence of elevation angles. The fourth SIRIS balloon flight was carried out from Palestine, Texas on September 15-16, 1986 with 9 hours of nighttime data (40 km). High quality data with spectral resolution 0.022 cm(exp -1), were obtained for numerous limb sequences. Fifteen stratospheric species have been identified to date from this flight: five species from the NO(sub y) family (HNO3, NO2, NO, ClONO2, N2O5), plus CO2, O3, H2O, N2O, CH4, CCl3F, CCl2F2, CHF2Cl, CF4, and CCl4. The nighttime values of N2O5, ClONO2, and total odd nitrogen have been measured for the first time, and compared to model results. Analysis of the diurnal variation of N2O5 within the 1984 and 1986 data sets, and of the 1984 ClONO2 measurements, were presented in the literature. The demonstrated ability of SIRIS to measure all the major NO(sub y) species, and therefore to determine the partitioning of the nitrogen family over a continuous diurnal cycle, is a powerful tool in the verification and improvement of photochemical modeling.

Kunde, V. G.↗
NASA NTRS1994

Laboratory measurements of polar stratospheric cloud rate parameters

It is now clear that heterogeneous reactions play an important role in controlling the concentration of ozone in the stratosphere. In this work, the loss of N2O5 on ice substrates has been studied in a flow reactor in an attempt to gain a more fundamental understanding of these reactions. The apparent reaction probability in this system was found to decrease as the substrate was exposed to N2O5. A model which corrected for the loss of surface sites was developed and although it appears to fit the data for a given experiment quite well, it is concluded that the loss of reactive sites is not the full explanation. In addition, the results of an experimental and modeling study suggest that reaction on the internal surface of the ice substrates is not a major loss mechanism for N2O5 in the current work.

Kenner, Rex D.↗
NASA NTRS1994

Three-dimensional model interpretation of NO(x) measurements from the lower stratosphere

A three-dimensional off-line chemistry transport model, driven by European Center for Medium-Range Forecasts winds and temperatures, is used to interpret measurements of NO and NO2 taken from the DC-8 during the second Airborne Arctic Stratospheric Expedition. The model was run in three configurations: gas phase chemistry alone, inclusion of the N2O5 aerosol reaction, and inclusion of both N2O5 and ClONO2 aerosol reactions. The run including the N2O5 aerosol reaction alone usually agreed best with measured NO(x)/NO(y) ratios in midlatitude air masses. The NO(x)/NO(y) ratios of the run with both aerosol reactions were always too low, while the gas phase ratios were usually too high, especially during March. All three simulations generated extremely low NO2/NO(y) ratios in air parcels that had spent several days or more in the polar night. Measured NO2/NO(y) ratios in these types of air masses were sometimes equally low but could also be considerably higher. Observed NO/NO2 ratios differed strongly from known theory.

Folkins, Ian↗