Monte Carlo analysis of uncertainty propagation in a stratospheric model. 1: Development of a concise stratospheric model

A concise model has been developed to analyze uncertainties in stratospheric perturbations, yet uses a minimum of computer time and is complete enough to represent the results of more complex models. The steady state model applies iteration to achieve coupling between interacting species. The species are determined from diffusion equations with appropriate sources and sinks. Diurnal effects due to chlorine nitrate formation are accounted for by analytic approximation. The model has been used to evaluate steady state perturbations due to injections of chlorine and NO(X)

Monte Carlo analysis of uncertainty propagation in a stratospheric model. 2: Uncertainties due to reaction rates

A concise stratospheric model was used in a Monte-Carlo analysis of the propagation of reaction rate uncertainties through the calculation of an ozone perturbation due to the addition of chlorine. Two thousand Monte-Carlo cases were run with 55 reaction rates being varied. Excellent convergence was obtained in the output distributions because the model is sensitive to the uncertainties in only about 10 reactions. For a 1 ppby chlorine perturbation added to a 1.5 ppby chlorine background, the resultant 1 sigma uncertainty on the ozone perturbation is a factor of 1.69 on the high side and 1.80 on the low side. The corresponding 2 sigma factors are 2.86 and 3.23. Results are also given for the uncertainties, due to reaction rates, in the ambient concentrations of stratospheric species

Influence of Aerosol Heating on the Stratospheric Transport of the Mt. Pinatubo Eruption

On June 15th, 1991 the eruption of Mt. Pinatubo (15.1 deg. N, 120.3 Deg. E) in the Philippines injected about 20 Tg of sulfur dioxide in the stratosphere, which was transformed into sulfuric acid aerosol. The large perturbation of the background aerosol caused an increase in temperature in the lower stratosphere of 2-3 K. Even though stratospheric winds climatological]y tend to hinder the air mixing between the two hemispheres, observations have shown that a large part of the SO2 emitted by Mt. Pinatubo have been transported from the Northern to the Southern Hemisphere. We simulate the eruption of Mt. Pinatubo with the Goddard Earth Observing System (GEOS) version 5 global climate model, coupled to the aerosol module GOCART and the stratospheric chemistry module StratChem, to investigate the influence of the eruption of Mt. Pinatubo on the stratospheric transport pattern. We perform two ensembles of simulations: the first ensemble consists of runs without coupling between aerosol and radiation. In these simulations the plume of aerosols is treated as a passive tracer and the atmosphere is unperturbed. In the second ensemble of simulations aerosols and radiation are coupled. We show that the set of runs with interactive aerosol produces a larger cross-equatorial transport of the Pinatubo cloud. In our simulations the local heating perturbation caused by the sudden injection of volcanic aerosol changes the pattern of the stratospheric winds causing more intrusion of air from the Northern into the Southern Hemisphere. Furthermore, we perform simulations changing the injection height of the cloud, and study the transport of the plume resulting from the different scenarios. Comparisons of model results with SAGE II and AVHRR satellite observations will be shown

Assessment of possible environmental effects of space shuttle operations

The potential of shuttle operations to contribute to atmospheric pollution is investigated. Presented in this interim report are results of the study to date on rocket exhaust inventory, exhaust interactions, dispersion of the ground cloud, detection and measurement of hydrochloric acid and aluminum oxide, environmental effects of hydrochloric acid and aluminum oxide, stratospheric effects of shuttle effluents, and mesospheric and ionospheric effects of orbiter reentry. The results indicate space shuttle operation will not result in adverse environmental effects if appropriate launch constraints are met

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%

Fast two-dimensional model

A two dimensional (altitude and latitude) model of the atmosphere is used to investigate problems relating to the variability of the dynamics and temperature of the atmosphere on the ozone distribution, solar cycle variations of atmospheric constituents, the sensitivity of model results to tropospheric trace gas sources, and assessment computations of changes in ozone related to manmade influences. In a comparison between two dimensional model results in which the odd nitrogen family was transported together and model results in which the odd nitrogen species was transported separately, it was found that the family approximations are adequate for perturbation scenario calculations

The Chemical and Dynamical Responses of Ozone and Nitrogen Dioxide to the Eruption of Mt. Pinatubo

Observations have shown that the concentration of nitrogen dioxide decreased in both hemispheres in the years following the eruption of Mt. Pinatubo. In contrast, the observed ozone response was largely asymmetrical with respect to the equator, with a decrease in the northern hemisphere and little or no change in the southern hemisphere. Simulations including enhanced heterogeneous chemistry due to the presence of the volcanic aerosol reproduce a decrease of ozone in the northern hemisphere, but also produce a comparable ozone decrease in the southern hemisphere contrary to observations. Our simulations show that the heating due to the volcanic aerosol enhanced both the tropical upwelling and the extratropical downwelling. The enhanced extratropical downwelling, combined with the time of the eruption relative to the seasonal phase of the Brewer-Dobson circulation, increased the ozone in the southern hemisphere and counteracted the ozone depletion due to heterogeneous chemistry on volcanic aerosol

Trends in total column ozone measurements

It is important to ensure the best available data are used in any determination of possible trends in total ozone in order to have the most accurate estimates of any trends and the associated uncertainties. Accordingly, the existing total ozone records were examined in considerable detail. Once the best data set has been produced, the statistical analysis must examine the data for any effects that might indicate changes in the behavior of global total ozone. The changes at any individual measuring station could be local in nature, and herein, particular attention was paid to the seasonal and latitudinal variations of total ozone, because two dimensional photochemical models indicate that any changes in total ozone would be most pronounced at high latitudes during the winter months. The conclusions derived from this detailed examination of available total ozone can be split into two categories, one concerning the quality and the other the statistical analysis of the total ozone record

Simulation of Long Lived Tracers Using an Improved Empirically Based Two-Dimensional Model Transport Algorithm

We have developed a new empirically-based transport algorithm for use in our GSFC two-dimensional transport and chemistry model. The new algorithm contains planetary wave statistics, and parameterizations to account for the effects due to gravity waves and equatorial Kelvin waves. As such, this scheme utilizes significantly more information compared to our previous algorithm which was based only on zonal mean temperatures and heating rates. The new model transport captures much of the qualitative structure and seasonal variability observed in long lived tracers, such as: isolation of the tropics and the southern hemisphere winter polar vortex; the well mixed surf-zone region of the winter sub-tropics and mid-latitudes; the latitudinal and seasonal variations of total ozone; and the seasonal variations of mesospheric H2O. The model also indicates a double peaked structure in methane associated with the semiannual oscillation in the tropical upper stratosphere. This feature is similar in phase but is significantly weaker in amplitude compared to the observations. The model simulations of carbon-14 and strontium-90 are in good agreement with observations, both in simulating the peak in mixing ratio at 20-25 km, and the decrease with altitude in mixing ratio above 25 km. We also find mostly good agreement between modeled and observed age of air determined from SF6 outside of the northern hemisphere polar vortex. However, observations inside the vortex reveal significantly older air compared to the model. This is consistent with the model deficiencies in simulating CH4 in the northern hemisphere winter high latitudes and illustrates the limitations of the current climatological zonal mean model formulation. The propagation of seasonal signals in water vapor and CO2 in the lower stratosphere showed general agreement in phase, and the model qualitatively captured the observed amplitude decrease in CO2 from the tropics to midlatitudes. However, the simulated seasonal amplitudes were attenuated too rapidly with altitude in the tropics. Overall, the simulations with the new transport formulation are in substantially better agreement with observations compared with our previous model transport

The global distribution of ozone destruction rates obtained from 13 years of Nimbus/TOMS data (1979-1991)

Long-term ozone trends (percentage change) have been computed from 13 years of Nimbus/TOMS (Total Ozone Mapping Spectrometer) data as a function of latitude, longitude, and month for the period January 1, 1979 to December 31, 1991. In both hemispheres, the ozone column content has decreased at latitudes above 30 deg by amounts that are larger than predicted by homogeneous chemistry models for the 13-year time period. The largest rates of ozone decrease occur in the Southern Hemisphere during winter and spring, with recovery during the summer and autumn. The large winter ozone loss rates are consistent with observed low stratospheric temperatures, ice-cloud formation, and heterogeneous chemistry at middle and high latitudes. There are similar, but smaller changes observed in the Northern Hemisphere. At midlatitudes, (40 deg N to 50 deg N) there are increased zonal average ozone depletion rates that correspond to 5 geographically localized regions of increased ozone depletion rates. Only the equatorial band between plus or minus 20 deg shows little or no long-term ozone change since January, 1979. The long-term winter ozone depletion rate data for both hemispheres suggests that heterogeneous chemistry processes may operate over a wide range of latitudes during half of the year