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At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
NASA NTRS1987

Response of middle atmosphere to short-term solar ultraviolet variations. I - Observations. II - Theory

The effects of solar UV variability on ozone and temperature are studied using Nimbus 7 stratospheric and mesospheric ozone, temperature, and 205-nm solar UV data, and Solar Mesosphere Explorer 1.27-micron ozone and 121.6-nm solar UV data. Consideration is given to the temperature/UV relation, the O3/UV relation with and without temperature feedback, and the responses of HNO3 and NO2 to solar UV variability. It is observed that the response times of temperature to solar UV variability are 6 days at 2 mbar and 1 day at 0.01 mbar. The stratospheric ozone response (with no correction for temperature effects) increases, while in the mesosphere a decrease is detected. The responses of ozone and temperature to solar variability are examined and calculated using a one-dimensional chemical-radiative time-dependent model. The comparison of the model results with the satellite-observed responses reveals generally good correlation between the data; however, the model predicts a larger time lag of the temperature response and a larger stratospheric HNO3 mixing ratio than the satellite data. It is noted that the relation between short-term variations in the solar UV radiation and stratospheric ozone is affected by the coupling between ozone and temperature.

Keating, G. M.↗
NASA NTRS1987

Nitric acid forecast experiments

Results of two three-dimensional forecasts of the time evolution of the distribution of HNO3 in the stratosphere are reported. The first is for the February 1979 stratospheric warming, and the second is for a period in March, 1979 when the relative importance of photochemistry and dynamics is thought to be rapidly changing. The zonal mean results of the model calculations are in general qualitative agreement with the LIMS HNO3 observations. However, the calculated three-dimensional fields show significant differences from the observations. The results provide insight into what must be done to form a successful constituent forecast model and provide information on the modeling technique and the self-consistency of the observed dynamical and constituent fields.

Rood, Richard B.↗
NASA NTRS1987

Antarctic stratospheric chemistry of chlorine nitrate, hydrogen chloride, and ice - Release of active chlorine

The reaction rate between atmospheric hydrogen chloride (HCl) and chlorine nitrate (ClONO2) is greatly enhanced in the presence of ice particles; HCl dissolves readily into ice, and the collisional reaction probability for ClONO2 on the surface of ice with HCl in the mole fraction range from about 0.003 to 0.010 is in the range from about 0.05 to 0.1 for temperatures near 200 K. Chlorine is released into the gas phase on a time scale of at most a few milliseconds, whereas nitric acid (HNO3), the other product, remains in the condensed phase. This reaction could play an important role in explaining the observed depletion of ozone over Antarctica; it releases photolytically active chlorine from its most abundant reservoir species, and it promotes the formation of HNO3 and thus removes nitrogen dioxide from the gas phase. Hence it establishes the necessary conditions for the efficient catalytic destruction of ozone by halogenated free radicals.

Molina, Mario J.↗
NASA NTRS1988

Laboratory studies of sticking coefficients and heterogeneous reactions important in the Antarctic stratosphere

Laboratory studies of sticking coefficients of H2O, HCl, Cl2, and HNO3 on ice and heterogeneous reactions of ClONO2 with ice or HCl/ice have been performed in a fast flow reactor. A quadrupole mass spectrometer with electron impact ionization was used as a detector. Measured sticking coefficients are: 0.3 (+0.7, -0.1) for H2O, 0.4 (+0.6, -0.2) for HCL, less than 0.0001 for Cl2, and 0.3 (+0.7, -0.1) for HNO3 at 200 K. The reaction probability of ClONO2 on ice was found to be 0.06 (+ or - 0.03) while HOCl was observed as a sole product in the gas phase. With HCl present in ice, the reaction probability of ClONO2 is greatly enhanced, approaching 0.27 (+0.73, -0.13) while molecular chlorine was found to be the major product in the gas phase. Another reaction product was nitric acid which remained in the solid phase. Since the polar stratospheric clouds contain ice particles or possibly HCl/ice particles on the surface, the present results should be a major factor in producing the observed springtime ozone depletion in the Antarctic stratosphere.

Leu, Ming-Taun↗
NASA NTRS1988

Chemistry of the Antarctic stratosphere

Interferometric measurements of HCl, ClNO3, HNO3, NO2, and NO obtained over the Antarctic in 1986 are used to model the chemistry of the atmosphere in the region of the Ozone Hole. The low abundance noted in stratospheric HCl is attributed to incorporation of HCl in polar stratospheric clouds and subsequent reaction of HCl with ClNO3. The results point to a net loss of HNO3 from the stratosphere and to the suppression of the abundance of odd nitrogen at high altitudes in the vortex. O3 loss is suggested to be due to the catalytic influence of halogen radicals.

Mcelroy, Michael B.↗
NASA NTRS1988

Interactions between HCl, NO(x), and H2O ice in the Antarctic stratosphere - Implications for ozone

The role of PSC particles in determining the distributions of HCl and chlorine radicals is studied. The thermodynamics of HCl in ice is discussed, showing that significant quantities of HCl may be dissolved in ice when PSCs form. It is argued that HCl and HNO3 will be removed from the gas phase early in the condensation process, when only small quantities of H2O have been condensed, reflecting the thermodynamic properties of the solid phases of HCl, HNO3, and H2O. Rapid heterogeneous chemical reactions then volatilize reactive chlorine gases and convert NO(x) to solid-phase nitrates, which can be removed by gravitational settling. Analysis of the suite of heterogeneous chemical processes in the polar stratosphere implies a threshold for HCl concentrations, above which chemical loss rates for ozone increase dramatically.

Wofsy, S. C.↗
NASA NTRS1988

Antarctic ozone depletion chemistry - Reactions of N2O5 with H2O and HCl on ice surfaces

In a study concerning Antarctic ozone depletion, reactions of dinitrogen pentoxide with water and hydrochloric acid were studied on ice surfaces in a Knudsen cell flow reactor. The N2O5 reacted on ice at 185 K to form condensed-phase nitric acid (HNO3). This reaction may provide a sink for odd nitrogen, NO(x), during the polar winter, a requirement in nearly all models of Antarctic ozone depletion. The reaction of N2O5 on HCl-ice surfaces at 185 K produced gaseous nitryl chloride (ClNO2) and condensed-phase HNO3 and proceeded until all of the HCl within the ice was depleted. The ClNO2 which did not react or condense on ice at 185 K, can be readily photolyzed in the Antarctic spring to form atomic chlorine for catalytic ozone destruction cycles. The other photolysis product, gaseous nitrogen dioxide may be important in the partitioning of NO(x) between gaseous and condensed phases in the Antarctic winter.

Tolbert, Margaret A.↗
NASA NTRS1988

Nitric acid and ammonia emissions from a mid-latitude prescribed wetlands fire

The first simultaneous measurements of gaseous nitric acid and ammonia in the smoke plume of a wetlands biomass burn were obtained. The measurements were made using tungsten oxide-coated diffusion denuder tubes from a helicopter during a prescribed burn on November 9, 1987, at the Merritt Island National Wildlife Refuge, located at the NASA John F. Kennedy Space Center, Florida. The mean NH3 and HNO3 mixing ratios measured in the smoke plume were 19 ppbv and 14 ppbv, respectively, both significantly higher than background mixing ratios. Nitric acid correlated well with carbon dioxide produced by the combustion. The mean CO2-normalized emission ratio for HNO3 was found to be 0.00012. Ammonia, however, dit not correlate well with CO2, suggesting a more complex relationship between combustion and production/release of NH3.

Lebel, P. J.↗
NASA NTRS1988

Retrieval of constituent mixing ratios from limb thermal emission spectra

An onion-peeling iterative, least-squares relaxation method to retrieve mixing ratio profiles from limb thermal emission spectra is presented. The method has been tested on synthetic data, containing various amounts of added random noise for O3, HNO3, and N2O. The retrieval method is used to obtain O3 and HNO3 mixing ratio profiles from high-resolution thermal emission spectra. Results of the retrievals compare favorably with those obtained previously.

Shaffer, William A.↗
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

Infrared measurements in the spring 1987 ozone hole

Solar spectra were recorded from Arrival Heights (McMurdo), Antartica, with a FTIR system during the austral spring of 1987. Spectra were recorded on 22 days from September 13 through October 28. The instrument was setup with 2 detectors for simultaneous operation in 2 wavelength regions. Several stratospheric gases have measurable absorptions in these regions including HCl, HNO3, O3, ClONO2, and NO2. The system is equipped with an automatic solar tracking system and records data on tape cartridges. A portable personal computer allows Fourier transforming and initial processing of some of the data. The HNO3 gas column amount shows large variations, but no apparent correlation with stratospheric temperature. The HCl column shows a steady increase from 0.9 x 10 to the 15th power molecules/sq.cm. on September 13 to 1.5 x 10 to the 15th power on October 6. McMurdo moved out of the polar vortex for a few days, and the HCl column jumped to 2.9 x 10 to the 15th power by October 11. Although McMurdo moved back under the vortex, the HCl continued to increase, reaching 3.4 x 10 to the 15th power at the end of the period.

Murcray, F. J.↗
NASA NTRS1989

Airborne measurements of stratospheric constituents over Antarctica in the austral spring, 1987. II - Halogen and nitrogen trace gases

The IR absorption spectra of the polar stratosphere, recorded by a Fourier transform spectrometer aboard the NASA DC-8 aircraft during the Airborne Antarctic Ozone Experiment, were used to derive vertical column amounts above flight altitude of HCl, HF, NO, NO2, ClONO2, and HNO3 in the region of disturbed ozone chemistry during September 1987. Significant reductions in the amounts of HCl, NO, NO2, and HNO3 were observed within the confines of the polar vortex, compared with amounts outside the vortex. When compared with the springtime observations by the same instrument in the Northern Hemisphere, the HCl and NO2 species displayed the most dramatic depletions. The results obtained are generally in agreement with the earlier ground measurements conducted at the McMurdo Station.

Coffey, M. T.↗
NASA NTRS1990

Airborne measurements of stratospheric constituents over the Arctic in the winter of 1989

A Fourier transform spectrometer aboard the NASA DC-8 aircraft was used during the Airborne Arctic Stratospheric Expedition (AASE) to record infrared absorption spectra of the polar stratosphere. From these high resolution spectra, vertical column amounts above flight altitude were derived of O3, CH4, N2O, H2O, HCl, HF, NO, NO2, ClONO2, and HNO3 for eleven flights poleward of 60 deg N. In this paper, measurements on the flight of January 26, 1989 were derived when the flight path during the observations crossed from outside the polar vortex to inside. This allowed a clear comparison of the conditions of the air within the vortex with that outside. Observations of passive tracers such as CH4 and HF indicate that air of a certain composition within the polar vortex occurs at lower altitude than air outside. Within the vortex, markedly reduced columns of HCl and NO2. The ratio of HCl to HF column dropped from its typical midlatitude value of 4.5 to as low as 1.7 within the vortex, implying that the HCl had been chemically or physically removed from the air in the vortex. In contrast to the Antarctic observations, HNO3 values were elevated within the vortex.

Mankin, William G.↗
NASA NTRS1990

Operational overview of NASA GTE/CITE 2 airborne instrument intercomparisons - Nitrogen dioxide, nitric acid, and peroxyacetyl nitrate

This paper provides the rationale, objectives, approach, and a brief description of the instrumentation included in the second airborne Chemical Instrumentation Test and Evaluation (CITE 2) mission conducted on NASA's Electra aircraft. CITE 2 intercompared data from instruments measuring NO2, HNO3, and PAN in the troposphere. This study, conducted in August 1986, encountered marine and continental air with free tropospheric mixing ratios of NO2, HNO3, and PAN typically less than 120, 150, and 200 parts per trillion by volume, respectively.

Hoell, James M., Jr.↗
NASA NTRS1990

An intercomparison of airborne nitric acid measurements

Results are reported on the performance of (1) denuder-tube/chemiluminescent, (2) nylon-filter/ion-chromatography, and (3) tunable-diode-laser/multipath-absorption HNO3 measurement instruments during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 (CITE 2) program in summer 1986. The instrument designs, test protocols, and CITE 2 flights are described, and the results are presented in extensive graphs and discussed in detail. The data obtained with the three instruments are shown to be in very poor agreement at mixing ratios below 150 parts per trillion by volume (pptv), with significant discrepancies even at higher levels. Instrument (3) gave systematically higher values than (1) and (2). It is concluded that none of the instruments is accurate enough for reliable use at normal atmospheric HNO3 levels (around 100 pptv).

Gregory, G. L.↗
NASA NTRS1991

Measurements in polar stratospheric clouds over Antarctica in September 1989

The results of six balloon flights at McMurdo Station, Antarctica, under varying temperature conditions, are used in a study of polar stratospheric clouds during Sept. 1989. A particle counter, with size resolution in the 0.5 micron radius region, indicates that cloud size distributions are always bimodal. Mode radii ranging from 0.05 to 0.10 microns were observed for the small particle mode, representing the sulfate layer or condensational growth enhancements of it. The data are not inconsistent with the expected increase in size with decreasing temperature of the small particle mode in the sulfate layer owing to deliquescence although this phenomenon is often masked by nitric acid trihydrate (NAT) condensation when temperatures are sufficiently low. Mode radii generally ranged from 1.5 to 3.5 micron for the large particle mode at concentrations 3 to 4 orders of magnitude lower than the small particle mode. The large particle mode, which normally comprises most of the mass, is presumably caused by NAT condensation on larger particles of the sulfate layer and indicates HNO3 mixing ratios of 1 to 5 ppbv for most of the cloud layers observed, suggesting substantial denitrification. On several occasions, distributions were observed with mode radii as high as 7 microns, and correspondingly large inferred mass, indicating water ice clouds in the 12 to 15 km region. On other occasions, absence of such clouds at very low temperatures indicated water vapor mixing ratios of less than 3 ppmv suggesting dehydration. Generally, the inferred HNO3 mixing ratios were higher in the lower stratosphere, suggesting redistribution through particle sedimentation.

Deshler, Terry↗
NASA NTRS1990

Fourier transform infrared studies of model polar stratospheric cloud surfaces - Growth and evaporation of ice and nitric acid/ice

Fourier-transform infrared surface studies are used to probe the microphysical properties of nitric acid trihydrate (NAT) and ice films representative of type I and II polar stratospheric clouds (PSC). Experiments indicate that, on initial exposure to 1.8 microtorr of HNO3, a layer of ice is quantitatively converted to NAT. However, conversion of ice to NAT does not proceed indefinitely, but rather the system reaches saturation. For longer exposures or higher HNO3 pressures, NAM becomes the dominant nitric acid containing species on the surface. Evaporation studies were performed to test the feasibility of a recent denitrification mechanism. The results indicate that ice coated with 0.20 micron of NAT evaporates at a temperature of about 4 C higher than uncoated ice.

Tolbert, Margaret A.↗
NASA NTRS1991

Heterogeneous reactions with NaCl in the El Chichon volcanic aerosols

Previous investigations of the effects of the 1982 eruption of the El Chichon volcano could not explain all the observations of changes in O3, HCl, NO and NO2 simultaneously without proposing unproven chemical reactions. Since reactions between solid NaCl and gaseous ClNO3 and N2O5 rapidly produce photochemically active chlorine species and solid NaNO3 in laboratory experiments, it is suggested that these reactions could have occurred with the NaCl observed to be present in the El Chichon sulfuric acid areosols. As a consequence, it is predicted that HCl should increase substantially, while NO(x) should decrease, in agreement with the measurements after the eruption. Ozone should be only slightly affected by these reactions. Reactions between solid NaCl and the acids H2SO4 and HNO3 might prove to be important, but sufficient evidence regarding their efficiency and the pressure of HNO3 in the aerosols is lacking.

Michelangeli, Diane V.↗