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Stolarski, R. S.

Publications and source records attributed to Stolarski, R. S..

At least 55 records · Page 3

Trends in stratospheric minor constituents

Photochemical models predict that increasing source gas concentrations are also expected to lead to changes in the concentrations of both catalytically active radical species (such as NO2, ClO, and OH) and inactive reservoir species (such as HNO3, HCl, and H2O). For simplicity, we will refer to all these as trace species. Those species that are expected to have increasing concentration levels are investigated. Additionally, the trace species concentration levels are monitored for unexpected changes on the basis of the measure increase in source gases. Carrying out these investigations is difficult due to the limited data base of measurements of stratospheric trace species. In situ measurements are made only infrequently, and there are few satelliteborne measurements, most over a time space insufficient for trend determination. Instead, ground-based measurements of column content must be used for many species, and interpretation is complicated by contributions from the troposphere or mesosphere or both. In this chapter, we examine existing measurements as published or tabulated.

Stolarski, R. S.↗

TOMS observations of total ozone in the 1986 Antarctic spring

Total ozone measurements by the Total Ozone Mapping Spectrometer (TOMS) aboard the Nimbus 7 satellite show the reappearance in 1986 of the extreme springtime Antarctic ozone minimum during September and October.The minimum total ozone amounts descended to 156 Dobson Units; the minimum October average of 185 DU was 27 DU higher than the corresponding average in 1985 and 5 DU less than the 1984 average. This behavior indicates a pause in the downward trend of recent years.

Krueger, A. J.↗

Nimbus 7 satellite measurements of the springtime Antarctic ozone decrease

Measurements from the Solar Backscatter Ultraviolet instrument and the Total Ozone Mapping Spectrometer aboard the Nimbus 7 satellite, a sun-synchronous polar-orbiting satellite which passes any given point on the dayside near local noon, are reported. These provide global measurements of ozone from November 1978 to the present which confirm the reported decline in total ozone in the Antarctic region and show the phenomenon to be regional in extent. The decrease occurs during September as the sun rises, reaching a minimum in mid-October. Seven years (1979-1985) of October monthly means show a 40 percent decrease in the ozone minimum and a 20 percent decrease in the surrounding ozone maximum.

Stolarski, R. S.↗

Sensitivity of an atmospheric photochemistry model to chlorine perturbations including consideration of uncertainty propagation

Models of stratospheric photochemistry are generally tested by comparing their predictions for the composition of the present atmosphere with measurements of species concentrations. These models are then used to make predictions of the atmospheric sensitivity to perturbations. Here the problem of the sensitivity of such a model to chlorine perturbations ranging from the present influx of chlorine-containing compounds to several times that influx is addressed. The effects of uncertainties in input parameters, including reaction rate coefficients, cross sections, solar fluxes, and boundary conditions, are evaluated using a Monte Carlo method in which the values of the input parameters are randomly selected. The results are probability distributions for present atmosheric concentrations and for calculated perturbations due to chlorine from fluorocarbons. For more than 300 Monte Carlo runs the calculated ozone perturbation for continued emission of fluorocarbons at today's rates had a mean value of -6.2 percent, with a 1-sigma width of 5.5 percent. Using the same runs but only allowing the cases in which the calculated present atmosphere values of NO, NO2, and ClO at 25 km altitude fell within the range of measurements yielded a mean ozone depletion of -3 percent, with a 1-sigma deviation of 2.2 percent. The model showed a nonlinear behavior as a function of added fluorocarbons. The mean of the Monte Carlo runs was less nonlinear than the model run using mean value of the input parameters.

Stolarski, R. S.↗

Present state of knowledge of the upper atmosphere: An assessment report; processes that control ozone and other climatically important trace gases

The state of knowledge of the upper atmosphere was assessed as of January 1986. The physical, chemical, and radiative processes which control the spatial and temporal distribution of ozone in the atmosphere; the predicted magnitude of ozone perturbations and climate changes for a variety of trace gas scenarios; and the ozone and temperature data used to detect the presence or absence of a long term trend were discussed. This assessment report was written by a small group of NASA scientists, was peer reviewed, and is based primarily on the comprehensive international assessment document entitled Atmospheric Ozone 1985: Assessment of Our Understanding of the Processes Controlling Its Present Distribution and Change, to be published as the World Meteorological Organization Global Ozone Research and Monitoring Project Report No. 16.

Watson, R. T.↗

Two-dimensional monthly average ozone balance from limb infrared monitor of the stratosphere and stratospheric and mesospheric sounder data

For many years, atmospheric scientists have been concerned with the balance of ozone production and loss terms in the upper stratosphere. Crutzen and Schmailzl (1983) found that the ozone loss was higher than the ozone production in the upper stratosphere. In the present investigation, previous studies are used as a basis in the conduction of a two-dimensional calculation of the production and loss of ozone. The monthly and zonally averaged loss and production rates for ozone are computed using recent Nimbus 7 satellite measurements of stratospheric constituents and accepted reaction and photodissociation rates. It is found that ozone has a loss rate which is about 40-60 percent higher than the production in the photochemical region.

Jackman, C. H.↗

Interpretation of ozone temperature correlations. II - Analysis of SBUV ozone data

In an effort to understand the behavior of ozone in the transition region, the terms in the perturbation continuity equation have been evaluated from solar backscattered ultraviolet ozone data, National Meteorological Center temperature data, and geostrophic winds derived from the temperature data at 2 mbar, winter 1978-1979. A linear parameterization is used to estimate the chemical source term. The perturbation ozone field calculated by integrating the net forcing evaluated from the data compares well with the measured perturbation ozone field. There are occasions during the winter when the sum of the dynamic terms is small due to cancellation, and the ozone and temperature perturbations are anticorrelated. The -1 correlation between the ozone and temperature perturbations does not necessarily imply that chemical forcing is dominant.

Douglass, A. R.↗

Parameterization of the photochemistry of stratospheric ozone including catalytic loss processes

A parameterization has been developed which accurately describes the photochemical response of odd oxygen to dynamically induced perturbations in odd oxygen and temperature. The temperature and odd oxygen dependencies of the loss processes for odd oxygen through catalytic cycles involving odd nitrogen, odd chlorine, and odd hydrogen have been specifically included. The assumption that a linear perturbation equation may be used to describe the response of odd oxygen to perturbations in odd oxygen and temperature has been tested and found to be acceptable for a physically reasonable range of perturbations, i.e., up to approximately 50 percent in odd oxygen mixing ratio and approximately 10 K in temperature. The scheme should prove useful for analyzing the feedback between ozone chemistry and ozone transport and also for analysis of ozone and temperature data.

Stolarski, R. S.↗

Production of odd nitrogen in the stratosphere and mesosphere - An intercomparison of source strengths

Galactic cosmic rays (GCRs), nuclear explosions, lightning, solar proton events (SPEs), relativistic electron precipitation, and meteors are related to the oxidation of nitrous oxide by comparing several sources of odd nitrogen (ON) in the stratosphere and mesosphere. Published O3 and N2O data show that ON produced by the reaction of O(1D) with N2O peaks between 25 and 35 km; the GCRs add approximately the same amount of ON as N2O oxidation at the solar minimum for geographic latitudes over 50 deg. Nuclear explosions in 1961-1962 added 1.1 and 2.2 x 10 to the 34th NO molecules each, and SPEs produced greater amounts of ON above 50 deg than N2O oxidation during 1958 through 1960, and in 1972.

Jackman, C. H.↗

Possible effects of volcanic eruptions on stratospheric minor constituent chemistry

Although stratosphere penetrating volcanic eruptions have been infrequent during the last half century, periods have existed in the last several hundred years when such eruptions were significantly more frequent. Several mechanisms exist for these injections to affect stratospheric minor constituent chemistry, both on the long-term average and for short-term perturbations. These mechanisms are reviewed and, because of the sensitivity of current models of stratospheric ozone to chlorine perturbations, quantitative estimates are made of chlorine injection rates. It is found that, if chlorine makes up as much as 0.5 to 1% of the gases released and if the total gases released are about the same magnitude as the fine ash, then a major stratosphere penetrating eruption could deplete the ozone column by several percent. The estimate for the Agung eruption of 1963 is just under 1% an amount not excluded by the ozone record but complicated by the peak in atmospheric nuclear explosions at about the same time.

Stolarski, R. S.↗

The reaction Cl + H2CO yields HCl + HCO: Decreased sensitivity of stratospheric ozone to chlorine perturbations

The absolute rate constant for the reaction Cl + H2CO yields HCl + HCO has been determined by the flash-photolysis-resonance fluorescence method to be + or - 0.9 (2 sigma) x 10 to the -11th power cu cm/molecule per sec at 298 K and to have a negligible temperature dependence. This rate, which at stratospheric temperatures is more than 2000 times faster than the rate of Cl + CH4 and more than a factor of 2 faster than Cl + HO2, indicates that formaldehyde (H2CO) will compete significantly with methane (CH4) and HO2 for the conversion of active chlorine in the stratosphere to the inactive reservoir HCl. Chlorine will thus be a less efficient destroyer of stratospheric ozone than previously believed. One-dimensional eddy-diffusion photochemical model calculations indicate that the eventual ozone depletion for a steady-state chlorfluoromethane release at 1975 rates (750,000 tons/year) will be lowered from 20% to 18.5% by the inclusion of this reaction.

Stief, L. J.↗

Uncertainty propagation in a stratospheric model. I - Development of a concise stratospheric model. II - Monte Carlo analysis of imprecisions due to reaction rates

The paper discusses the development of a concise stratospheric model which uses iteration to obtain coupling between interacting species. The one-dimensional, steady-state, diurnally-averaged model generates diffusion equations with appropriate sources and sinks for species odd oxygen, H2O, H2, CO, N2O, odd nitrogen, CH4, CH3Cl, CCl4, CF2Cl2, CFCl3, and odd chlorine. The model evaluates steady-state perturbations caused by injections of chlorine and NO(x) and may be used to predict ozone depletion. The model is used in a Monte Carlo study of the propagation of reaction-rate imprecisions by calculating an ozone perturbation caused by the addition of chlorine. Since the model is sensitive to only 10 of the more than 50 reaction rates considered, only about 1000 Monte Carlo cases are required to span the space of possible results.

Rundel, R. D.↗

The reaction Cl + H2CO yields HCl + HCO: Decreased sensitivity of stratospheric ozone to chlorine perturbations

The absolute rate constant for the reaction Cl + H2CO yields HCl + HCO was determined by the flash-photolysis resonance fluorescence method to be 7.5 plus or minus 0.9 (2 sigma) times 10 to the minus 11th power cu cm/molecule sec at 298 K and to have a negligible temperature dependence. This rate which is more than 2000 times faster than the rate of Cl + CH4 indicates that formaldehyde (H2CO) will compete significantly with methane (CH4) for the conversion of active chlorine in the stratosphere to the inactive reservoir HCl. Chlorine will thus be a less efficient destroyer of stratosphere ozone than previously believed. Ambient stratospheric ozone will depend less on the ambient chlorine amount and the predicted response to chlorine perturbations will be lessened. One-dimensional eddy-diffusion photochemical model calculations indicate a factor of 1.1 less sensitivity to chlorine than recently reported. For a steady-state CFM release at 1975 rates (750,000 tons/year) the eventual ozone depletion is now calculated to be 14%.

Stief, L. J.↗