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Sze, N. D.

Publications and source records attributed to Sze, N. D..

36 records · Page 2

Profiles of Stratospheric Chlorine Nitrate from ATMOS/ATLAS 1 Infrared Solar Occultation Spectra

Stratospheric volume mixing ration profiles of chlorine nitrate have been retrieved from 0.01-cm(sub -1) resolution infrared solar occutation spectra recorded at latitudes between 14 degrees N and 54 degrees S by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the ATLAS 1 shuttle mission (March 24 to April 2, 1992).

chlorine nitrate ATMOS/ATLAS spectroscopic paramet

Infrared measurements of HF and HCl total column abundances above Kitt Peak, 1977-1990 - Seasonal cycles, long-term increases, and comparisons with model calculations

The paper deals with hydrogen-chloride and hydrogen-fluoride total column measurements, their estimated long-term rates of increase, seasonal cycles, and variability, deduced from the analysis of a set of high-resolution infrared solar spectra recorded at Kitt Peak. The Kitt Peak observations and methods of analysis are described, the results are presented and compared with previously reported measurements and trends. The data is analyzed by using a multilayer nonlinear least-squares spectral fitting procedure and a consistent set of spectroscopic line parameters. Model-calculated hydrogen-chloride and hydrogen-fluoride total columns obtained with a two-dimensional model are discussed, and the model results are compared with the measured hydrogen-chloride and hydrogen-fluoride total columns, seasonal cycles, and trends. It is pointed out that the observed trends of both molecules are in satisfactory agreement with the model results calculated from emission histories and photooxidation rates for the source molecules.

Rinsland, C. P.

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.

Nitrogen and chlorine species in the spring Antarctic stratosphere - Comparison of models with Airborne Antarctic Ozone Experiment observations

The concentrations and the time development of chlorine and nitrogen trace gases in the Antarctic stratosphere before, during, and after the Airborne Antractic Ozone Experiment (AAOE) were simulated using photochemical models of the Antractic stratosphere during winter/spring. The initial conditions in the calculations were constrained using observations by the AAOE instrument. The comparison of calculated results with the AAOE measurements of HCl and ClO suggest that heterogeneous chemistry was maintained throughout the month of September 1987.

Rodriguez, J. M.

Implications of AAOE observations for proposed chemical explanations of the seasonal and interannual behavior of Antarctic ozone

Model simulations were used to investigate the seasonal and interannual behavior of ozone for different choices of initial odd nitrogen concentration in July and different assumptions on the heterogeneous reactions, with particular consideration given to the possible contribution of chlorine chemistry to the ozone hole phenomenon. The numerical experiments were selected based on the simulations of the observed trace gas concentrations during the Airborne Antarctic Ozone Experiment in 1987. In all cases considered, the catalytic cycle associated with the formation and photolysis of Cl2O2 could account for more than half of the photochemical removal of O3 within the Antarctic vortex through mid-September. The reaction of BrO with ClO, which accounts for 15-20 percent of O3 removal in the same period, tends to play a more important role toward the end of September, when the concentration of ClO is expected to decrease. No simple relationship was found between the increase in chlorine lavel and the interannual decrease in Antarctic O3.

Ko, M. K. W.

Antarctic ozone hole - Possible implications for ozone trends in the Southern Hemisphere

Satellite-borne instruments (the Total Ozone Mapping Spectrometer and the Solar Backscattered Ultraviolet Instrument) show that, compared to 1979, total column ozone has a year-round decrease of more than 5 percent in the neighborhood of 60 deg S. The meteorological conditions (warmer temperatures, the absence of polar stratospheric clouds) at these latitudes do not seem to favor heterogeneous chemistry as the direct cause for the observed year-round ozone reduction. A mechanism involving the seasonal transport of ozone-poor air from within the polar vortex to lower latitudes (the so-called 'dilution effect') is proposed as a possible explanation for the observed year-round ozone reduction in subpolar regions. A two-dimensional model with an imposed springtime Antarctic ozone depletion is used to study the post-ozone hole impact on the spatial and temporal distributions of column ozone at latitudes north of 60 deg S. It is found that the time constant associated with the dilution effect in the latitude region 40-60 deg S is about 1 year, long enough to contribute to the observed year-round decrease of total ozone in that region.

Sze, N. D.

Are Antarctic ozone variations a manifestation of dynamics or chemistry?

The existence of a reverse circulation cell with rising motion in the polar lower stratosphere is suggested as an explanation for the temporal behavior of the ozone column density in the Antarctic region. The upwelling brings ozone-poor air from below 100 mbar to the stratosphere, possibly contributing to the observed ozone decline in early spring. At the same time, the Antarctic stratosphere might contain a very low concentration of NO(x), a condition that could favor a greatly enhanced catalytic removal of O3 by halogen species. It is argued that heterogeneous processes and formation of OClO by the reaction BrO+ClO - OClO+Br before and after the polar night might help to suppress the NO(x) levels during the early spring period.

Tung, K.-K.

Halogentated species

Stratospheric measurements of halogen containing species are reviewed and compared with model predictions. Halocarbons, HCl, HF, ClONO2, and ClO are discussed.

Molina, M. J.

Model predictions of ozone changes

The predictions of several one-dimensional models were examined for a number of prescribed scenarios in steady-state or time-dependent approximations. A small number of two-dimensional steady-state calculations for a limited number of scenarios were compared with the results of one-dimensional models. The sensitivity of the calculated predictions to the values of input parameters were examined in order to assess recognized uncertainties in these predictions.

Johnston, H. S.

Stratospheric chemistry

Recent improvements in the data base for the currently identified reactions describing the chemistry of the major families of trace gas species, HO(x), NO(x), ClO(x), and hydrocarbons are assessed. The important coupling reactions between the families are introduced progressively. Chemical aspects such as heterogeneous reactions and reactions of sodium species, the importance of which are not yet completely established, are discussed. Recent attempts to reconcile some of the more unexpected kinetic behavior which has emerged from the extensive experimental studies of key reactions with current reaction rate theory are also examined. The uncertainties in the current kinetic and photochemical data base is given. The prospects for improvement of data for known reactions of atmospheric importance as well as for the identification of gaps in the chemical description of the atmosphere.

Cox, R. A.

Atmospheric studies related to aerospace activities and remote sensing technology

Parallel investigations were conducted relating to: the sensitivity of 1-D photochemical model simulated column ozone perturbations due to a projected fleet of 1000 aircraft cruising 7 hours per day at altitudes of 15-16 and 18-19 km to uncertainties in kinetic rate constant data determining modeled OH concentrations and eddy diffusivity profile parameterization and a comparison of the inherent strengths and weaknesses of Eulerian and Langrangian averaging processes in the development of multidimensional models and investigation of approaches to applying the Generalized Lagrangian Mean (GLM) formalism to zonal-mean models. The role of multiple scattering and Earth curvature in the evaluation of diurnally dependent photodissociation rates and trace species variations was examined.

Sze, N. D.

Coupled effects of atmospheric N2O and O3 on the earth's climate

Increased application of nitrogen fertilizer could perturb the atmospheric nitrogen cycle and might lead to a possible increase in atmospheric N2O. N2O has an important role in stratospheric chemistry as well as in the global radiation budget. Recent studies suggest that perturbation of local ozone could also significantly affect the global climate. It is shown that a doubling in the present day N2O level might significantly perturb the distribution of O3 and HNO3, and that the associated climatic feedbacks from O3 and HNO3 perturbations could contribute as much as 0.23 K warming of the surface temperature, in addition to 0.44 K directly caused by N2O doubling.

Wang, W.-C.

The chemistry of Venus' atmosphere

A model for the Venus atmosphere involving photochemistry of oxygen, hydrogen, chlorine and sulfur species is presented. Sulfur reaction schemes and hydrogen and chlorine reaction schemes were included. The impact of sulfur on the oxygen budget and the subsequent production of H2SO4 molecules for the Venus cloud deck were explored. A major new reaction scheme for production of H2SO4 molecules involving sulfur and oxygen chemistry was established shown to dominate over the odd hydrogen scheme proposed earlier. The efficiency of the scheme in formation of H2SO4 is only about 50%, with the remaining sulfur residing in SO2 molecules. The calculated downward flux of H2SO4 may be sufficient to maintain a steady state sulfuric acid cloud if the resident time of H2SO4 droplets in the cloud is as long as a few years. If however, the resident time is half a year or shorter, additional chemistry capable of more efficient conversion of SO2 to SO3 is required.

Sze, N. D.

The development of a model to infer precipitation from microwave measurements

To permit the inference of precipitation amounts from radiometric measurements, a radiative interaction model was developed. This model uses a simple computational scheme to determine the effects of rain upon brightness temperatures and can be used with a statistical inversion procedure to invert for rain rate. Precipitating cloud models was also developed and used with the microwave model for frequencies of 19.35 and 37 GHz to determine the variability of the microwave-rain rate relationship on a global and seasonal basis.

Fowler, M. G.

Freon consumption - Implications for atmospheric ozone

Freons are a potential source of stratospheric chlorine and may indirectly cause serious reductions in the concentration of ozone. The reduction could be as large as 3 percent by 1980, or 16 percent by 2000, if Freon consumption were to grow at 10 percent per year. Even if Freon use were terminated as early as 1990, it could leave a significant effect which might endure for several hundred years.

Wofsy, S. C.

Venus cloud models

Remote observations of Venus are reviewed. The strongest inferences of cloud properties can be drawn from polarization data which provide information about cloud particles near 68 km. Particle properties are not as well determined at higher and lower levels. If the clouds are generated photochemically from reduced sulfur species, the supply of O2 may be an important constraint on cloud production. Vapor-pressure data reviewed, and it is shown that deep clouds cannot be H2SO4-H2O aerosols unless the mixing ratios of both H2SO4 and H2O approach 0.001 below 50 km.

Wofsy, S. C.