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The spatial and temporal variation in ozone production over major source regions in East Asia during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) measurement campaign in spring 2001 is assessed using a global chemical transport model. There is a strong latitudinal gradient in ozone production in springtime, driven by regional photochemistry, which rapidly diminishes as the season progresses. The great variability in meteorological conditions characteristic of East Asia in springtime leads to large daily variability in regional ozone formation, but we find that it has relatively little impact on the total global production. We note that transport processes effectively modulate and thus stabilize total ozone production through their influence over its location. However, the impact on the global ozone burden, important for assessing the effects of precursor emissions on tropospheric oxidizing capacity and climate, is sensitive to local meteorology through the effects of location on chemical lifetime. Stagnant, anticyclonic conditions conducive to substantial boundary layer ozone production typically allow little lifting of precursors into the free troposphere where greater ozone production could occur, and the consequent shorter chemical lifetime for ozone leads to relatively small impacts on global ozone. Conversely, cyclonic conditions with heavy cloud cover suppressing regional ozone production are often associated with substantial cloud convection, enhancing subsequent production in the free troposphere where chemical lifetimes are longer, and the impacts on global ozone are correspondingly greater. We find that ozone formation in the boundary layer and free troposphere outside the region of precursor emissions dominates total gross production from these sources in springtime, and that it makes a big contribution to the long range transport of ozone, which is greatest in this season.

Observations of CO and O3 from the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign are compared with modeled distributions from the FRSGC/UCI CTM driven by the Oslo T63L40 ECMWF forecast meteorology. The model-measurement comparison is made within the context of how well the TRACE-P observations represent the springtime chemistry and ozone distributions over eastern Asia and the western Pacific in March 2001 and uses the four-dimensional (4-D) extended domain from the model to provide unbiased statistics. A key question is whether the limited sampling density or mission strategy led to a statistically biased sample. To address this question, we examine a diverse range of statistical analyses of the observations of CO and O3. The middle percentiles of the cumulative probability functions for CO in the free troposphere are representative (and reproduced by the CTM), but those in the boundary layer are not. The frequency of low-CO, stratospheric influence is well matched along flight tracks but is atypical of the extended domain. The percentiles of the latitude-by-height distribution of lidar O3 show how the CTM reproduces the nonrepresentative clumpy nature of the observations but has too low a tropopause about the jet region (30–35N). Adaptive kernel estimation of the 2-D probability density of O3-CO correlations shows a very good simulation of two different chemical regimes (stratospheric and polluted) that is quite different from the extended domain but also highlights the failure to predict CO > 400 ppb. Empirical orthogonal function analysis of the O3 vertical profiles shows how six EOFs can effectively describe the 4-D structures of O3 over this entire domain. The latitude-by-longitude maps of the principal components provide an excellent test of the CTM simulation along flight tracks and clearly show the unique sampling of O3events by the TRACE-P flights. In many cases the ability of the model to simulate the nonrepresentative observations implies a clear skill in matching the unique meteorological and chemical features of the region.

Two closely related chemical transport models (CTMs) employing the same high-resolution meteorological data (∼180 km × ∼180 km × ∼600 m) from the European Centre for Medium-Range Weather Forecasts are used to simulate the ozone total column and tropospheric distribution over the western Pacific region that was explored by the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) measurement campaign in February–April 2001. We make extensive comparisons with ozone measurements from the lidar instrument on the NASA DC-8, with ozonesondes taken during the period around the Pacific Rim, and with TOMS total column ozone. These demonstrate that within the uncertainties of the meteorological data and the constraints of model resolution, the two CTMs (FRSGC/UCI and Oslo CTM2) can simulate the observed tropospheric ozone and do particularly well when realistic stratospheric ozone photochemistry is included. The greatest differences between the models and observations occur in the polluted boundary layer, where problems related to the simplified chemical mechanism and inadequate horizontal resolution are likely to have caused the net overestimation of about 10 ppb mole fraction. In the upper troposphere, the large variability driven by stratospheric intrusions makes agreement very sensitive to the timing of meteorological features.

Two sets of sea surface temperature/sea ice changes are used to test the sensitivity of tracer transport to the pattern of warming in the doubled CO2 climate. One set (2CO2WT) has greater tropical and high latitude sea surface temperature changes than the other (2CO2), although both fall within the range of plausible response. Simulations were done both with and without interactive ozone. Results show that the SST pattern affects the circulation change throughout the troposphere and middle atmosphere; the ozone interaction affects primarily the upper stratosphere, but through wave-mean flow interaction has effects that extend down into the upper troposphere. Both experiments feature increased tropospheric/stratospheric exchange at low latitudes and greater vertical mixing within the troposphere; only the WT experiments result in increased interhemispheric transport and a more direct circulation in the high latitude stratosphere. Ozone increases in the upper stratosphere and decreases in the lower stratosphere in all the simulations, with greater transport of high latitude ozone into the troposphere in the WT runs. At sea level there is a more positive phase of the Arctic Oscillation (AO)-type oscillation, and this is also true at 100 mbar, but there is no significance in the middle troposphere and the sign is different in the middle stratosphere. Many of these results differ from those generated in older versions of the GISS GCMAM despite the same SST forcing due to differences in control run characteristics, which has implications for model intercomparison experiments.

Radiative forcing due to changes in ozone is expected for the 21st century. An assessment on changes in the tropospheric oxidative state through a model intercomparison (“OxComp”) was conducted for the IPCC Third Assessment Report (IPCC-TAR). OxComp estimated tropospheric changes in ozone and other oxidants during the 21st century based on the “SRES” A2p emission scenario. In this study we analyze the results of 11 chemical transport models (CTMs) that participated in OxComp and use them as input for detailed radiative forcing calculations. We also address future ozone recovery in the lower stratosphere and its impact on radiative forcing by applying two models that calculate both tropospheric and stratospheric changes. The results of OxComp suggest an increase in global-mean tropospheric ozone between 11.4 and 20.5 DU for the 21st century, representing the model uncertainty range for the A2p scenario. As the A2p scenario constitutes the worst case proposed in IPCC-TAR we consider these results as an upper estimate. The radiative transfer model yields a positive radiative forcing ranging from 0.40 to 0.78 W m−2 on a global and annual average. The lower stratosphere contributes an additional 7.5–9.3 DU to the calculated increase in the ozone column, increasing radiative forcing by 0.15–0.17 W m−2. The modeled radiative forcing depends on the height distribution and geographical pattern of predicted ozone changes and shows a distinct seasonal variation. Despite the large variations between the 11 participating models, the calculated range for normalized radiative forcing is within 25%, indicating the ability to scale radiative forcing to global-mean ozone column change.

Two simple and computationally efficient models for simulating stratospheric ozone in three-dimensional global transport models are presented. The first, linearized ozone (or Linoz), is a first-order Taylor expansion of stratospheric chemical rates in which the ozone tendency has been linearized about the local ozone mixing ratio, temperature, and the overhead column ozone density. The second, synthetic ozone (or Synoz), is a passive, ozone-like tracer released into the stratosphere at a rate equivalent to that of the cross-tropopause ozone flux which, based on measurements and tracer-tracer correlations, we have calculated to be 475±120 Tg/yr. Linoz and Synoz have been evaluated in the UC Irvine chemical transport model (CTM) with three different archived meteorological fields: the Goddard Institute for Space Studies (GISS) general circulation model (GCM) version II′, the GISS GCM version II, and merged forecast data from the European Centre forecast model (EC/Oslo). Linoz produced realistic annual, cross-tropopause fluxes of 421 Tg/yr for the GISS II′ winds and 458 Tg/yr for the EC/Oslo winds; the GISS II winds produced an unrealistic flux of 790 Tg/yr. Linoz and Synoz profiles in the vicinity of the tropopause using the GISS II′ and EC/Oslo winds were found to be in good agreement with observations. We conclude that either approach may be adequate for a CTM focusing on tropospheric chemistry but that Linoz can also be used for calculating ozone fields interactively with the stratospheric circulation in a GCM. A future version of Linoz will allow for evolving background concentrations of key source gases, such as CH4 and N2O, and thus be applicable for long-term climate simulations.

A 3-D chemical transport model (OSLO CTM2) is used to investigate the impact of the increase of NO x emission over China. The model is capable to reproduce basically the seasonal variation of surface NO x and ozone over eastern China. NO x emission data and observations reveal that NO x over eastern China increases quite quickly with the economic development of China. Model results indicate that NO x concentration over eastern China increasingly rises with the increase of NO x emission over China, and accelerates to increase in winter. When the NO x emission increases from 1995 to its double, the ratio of NO2/NO x abruptly drops in winter over northern China. Ozone at the surface decreases in winter with the continual enhancement of the NO x level over eastern China, but increases over southern China in summertime. It is noticeable that peak ozone over northern China increases in summer although mean ozone changes little. In summer, ozone increases in the free troposphere dominantly below 500 hPa. Moreover, the increases of total ozone over eastern China are proportional to the increases of NO x emission. In a word, the model results suggest that the relationship between NO x and ozone at the surface would change with NO x increase. [ABSTRACT FROM AUTHOR]

A three-dimensional global chemistry transport model (OSLO CTM2) is used to investigate the impact of subsonic aircraft NO x emission on NO x and ozone over China in terms of a year 2000 scenario of subsonic aircraft NO x emission. The results show that subsonic aircraft NO x emission significantly affects northern China, which makes NO x at 250 hPa increase by about 50 pptv with the highest percentage of 60% in January, and leading to an ozone increase of 8 ppbv with 5% relative change in April. The NO x increase is mainly attributed to the transport process, but ozone increase is produced by the chemical process. The NO x increases by less than 10 pptv by virtue of subsonic aircraft NO x emission over China, and ozone changes less than 0.4 ppbv. When subsonic aircraft NO x emission over China is doubled, its influence is still relatively small. [ABSTRACT FROM AUTHOR]