[1] We present a global chemical transport model called the Integrated Massively Parallel Atmospheric Chemical Transport (IMPACT) model. This model treats chemical and physical processes in the troposphere, the stratosphere, and the climatically critical tropopause region, allowing for physically based simulations of past, present, and future ozone and its precursors. The model is driven by meteorological fields from general circulation models (GCMs) or assimilated fields representing particular time periods. It includes anthropogenic and natural emissions, advective and convective transport, vertical diffusion, dry deposition, wet scavenging, and photochemistry. Simulations presented here use meteorological fields from the National Center for Atmospheric Research (NCAR) Middle Atmospheric Community Climate Model, Version 3 (MACCM3). IMPACT simulations of radon/lead are compared to observed vertical profiles and seasonal cycles. IMPACT results for a full chemistry simulation, with approximately 100 chemical species and 300 reactions representative of a mid-1990s atmosphere, are presented. The results are compared with surface, satellite, and ozonesonde observations. The model calculates a total annual flux from the stratosphere of 663 Tg O 3 /year, and a net in situ tropospheric photochemical source (that is, production minus loss) of 161 Tg O 3 /year, with 826 Tg O 3 /year dry deposited. NO x is overpredicted in the lower midlatitude stratosphere, perhaps because model aerosol surface densities are lower than actual values or the NO x to NO y conversion rate is underpredicted. Analysis of the free radical budget shows that ozone and NO y abundances are simulated satisfactorily, as are HO x catalytic cycles and total production and removal rates for ozone.

Abstract. We describe a new parameterization of polar stratospheric clouds (PSCs) which was written for and incorporated into the three-dimensional (3-D) chemistry and transport model (CTM) developed for NASA's Atmospheric Effects of Aviation Project (AEAP) by the Global Modeling Initiative (GMI). The parameterization was designed to respond to changes in NO s and H20 produced by high-speed civilian transport (HSCT) emissions. The parameterization predicts surface area densities (SADs) of both Type 1 and Type 2 PSCs for use in heterogeneous chemistry calculations. Type 1 PSCs are assumed to have a supercooled ternary sulfate (STS) composition, and Type 2 PSCs are treated as water ice with a coexisting nitric acid trihydrate (NAT) phase. Sedimentation is treated by assuming that the PSC particles obey lognormal size distributions, resulting in a realistic mass flux of condensed phase H20 and HNO3. We examine a simulation of the Southern

The eruption of Mount Pinatubo introduced large amounts of sulfur‐containing particles into the stratosphere. Stratospheric ozone measured by ozonesondes and satellites is significantly lower following the June 1991 eruption and throughout 1992 and 1993. To clarify the mechanisms leading to effects on stratospheric ozone, time‐dependent stratospheric aerosol and gas experiment II (SAGE II) and cryogenic limb array elaton spectrometer (CLAES) aerosol optical extinction data and SAGE II surface area density are used as parameters in a two‐dimensional (2‐D) zonally averaged chemical radiative transport model. The model was integrated with time from before the eruption through December 1993. The modeled impact on global ozone results from increased rates of heterogeneous reactions on sulfate aerosols and from the increased radiative heating and scattering caused by these aerosols. The model's dynamical response to changes in forcing (from changes in radiatively active trace gas concentrations and from aerosol heating) is treated in one of three ways: (1) the stratospheric temperature is perturbed, with fixed seasonal circulation, (2) the circulation is perturbed, with fixed seasonal temperature, or (3) both circulation and temperature are unperturbed, when investigating only the impact of Mount Pinatubo increased aerosol surface area density (SAD) and aerosol scattering of actinic solar radiation, When the aerosol heating is allowed to modify the temperature distribution, the maximum change calculated in equatorial column ozone is −1.6%. The calculated equatorial temperature change and peak local ozone change in October 1991 are +6 K and −4%, respectively. When aerosol heating perturbs the circulation in the model, the maximum change in equatorial column ozone is −6%. Increased heterogeneous processing on sulfate aerosols is calculated to have changed equatorial column ozone in late 1991 by −1.5%. Global column ozone in the model in 1992 and 1993 changed by −2.8% and −2.4%, respectively. The relationship of ozone‐controlling processes in the lower stratosphere is altered as well; HOx becomes the most important catalytic cycle, followed by ClOx and NOx. This is driven by significant changes in trace gas concentrations. In October 1991, lower stratospheric, equatorial NOx decreased by 40%, ClOx increased by 60%, and HOx increased by 25%. When the effect of heterogeneous chemical processing on sulfate aerosols is combined with aerosol heating, modifying either circulation or temperature, dramatically different ozone fingerprints with time and latitude are predicted. Model‐derived changes in the equatorial region in column ozone best represented the observed data when perturbed circulation was combined with heterogeneous chemical effects. However, at high latitudes, the increased ozone production from the strengthening of the mean circulation tends to cancel the heterogeneous reduction of ozone. This is not in good agreement with observed data, especially in 1992 and 1993. When the circulation is held fixed and the tempe...

[1] We have used a three-dimensional chemistry and transport model (CTM), developed under the Global Modeling Initiative (GMI), to carry out two simulations of the composition of the stratosphere under changing halogen loading for 1995 through 2030. The two simulations differ only in that one uses meteorological fields from a general circulation model while the other uses meteorological fields from a data assimilation system. A single year's winds and temperatures are repeated for each 36-year simulation. We compare results from these two simulations with an extensive collection of data from satellite and ground-based measurements for 1993-2000. Comparisons of simulated fields with observations of radical and reservoir species for some of the major ozone-destroying compounds are of similar quality for both simulations. Differences in the upper stratosphere, caused by transport of total reactive nitrogen and methane, impact the balance among the ozone loss processes and the sensitivity of the two simulations to the change in composition.

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