Chemical nonlinearities in relating intercontinental ozone pollution to anthropogenic emissions

Model studies typically estimate intercontinental influence on surface ozone by perturbing emissions from a source continent and diagnosing the ozone response in the receptor continent. Since the response to perturbations is non-linear due to chemistry, conclusions drawn from different studies may depend on the magnitude of the applied perturbation. We investigate this issue for intercontinental transport between North America, Europe, and Asia with sensitivity simulations in three global chemical transport models. In each region, we decrease anthropogenic emissions of NOx and nonmethane volatile organic compounds (NMVOCs) by 20% and 100%. We find strong nonlinearity in the response to NOx perturbations outside summer, reflecting transitions in the chemical regime for ozone production. In contrast, we find no significant nonlinearity to NOx perturbations in summer or to NMVOC perturbations year-round. The relative benefit of decreasing NOx vs. NMVOC from current levels to abate intercontinental pollution increases with the magnitude of emission reductions

Characterizing the tropospheric ozone response to methane emission controls and the benefits to climate and air quality

Reducing methane (CH4) emissions is an attractive option for jointly addressing climate and ozone (O3) air quality goals. With multidecadal full-chemistry transient simulations in the MOZART-2 tropospheric chemistry model, we show that tropospheric O3 responds approximately linearly to changes in CH4 emissions over a range of anthropogenic emissions from 0–430 Tg CH4 a−1 (0.11–0.16 Tg tropospheric O3 or ∼11–15 ppt global mean surface O3 decrease per Tg a−1 CH4 reduced). We find that neither the air quality nor climate benefits depend strongly on the location of the CH4 emission reductions, implying that the lowest cost emission controls can be targeted. With a series of future (2005–2030) transient simulations, we demonstrate that cost-effective CH4 controls would offset the positive climate forcing from CH4 and O3 that would otherwise occur (from increases in NOx and CH4 emissions in the baseline scenario) and improve O3 air quality. We estimate that anthropogenic CH4 contributes 0.7 Wm−2 to climate forcing and ∼4 ppb to surface O3 in 2030 under the baseline scenario. Although the response of surface O3 to CH4 is relatively uniform spatially compared to that from other O3 precursors, it is strongest in regions where surface air mixes frequently with the free troposphere and where the local O3 formation regime is NOx-saturated. In the model, CH4 oxidation within the boundary layer (below ∼2.5 km) contributes more to surface O3 than CH4 oxidation in the free troposphere. In NOx-saturated regions, the surface O3 sensitivity to CH4 can be twice that of the global mean, with >70% of this sensitivity resulting from boundary layer oxidation of CH4. Accurately representing the NOx distribution is thus crucial for quantifying the O3 sensitivity to CH4

Impacts of climate change on surface ozone and intercontinental ozone pollution:a multi-model study

The impact of climate change between 2000 and 2095 SRES A2 climates on surface ozone (O)3 and on O3 source-receptor (S-R) relationships is quantified using three coupled climate-chemistry models (CCMs). The CCMs exhibit considerable variability in the spatial extent and location of surface O3 increases that occur within parts of high NOx emission source regions (up to 6 ppbv in the annual average and up to 14 ppbv in the season of maximum O3). In these source regions, all three CCMs show a positive relationship between surface O3 change and temperature change. Sensitivity simulations show that a combination of three individual chemical processes(i) enhanced PAN decomposition, (ii) higher water vapor concentrations, and (iii) enhanced isoprene emission largely reproduces the global spatial pattern of annual-mean surface O3 response due to climate change (R2=0.52). Changes in climate are found to exert a stronger control on the annual-mean surface O3 response through changes in climate-sensitive O3 chemistry than through changes in transport as evaluated from idealized CO-like tracer concentrations. All three CCMs exhibit a similar spatial pattern of annual-mean surface O3 change to 20% regional O3 precursor emission reductions under future climate compared to the same emission reductions applied under present-day climate. The surface O3 response to emission reductions is larger over the source region and smaller downwind in the future than under present-day conditions. All three CCMs show areas within Europe where regional emission reductions larger than 20% are required to compensate climate change impacts on annual-mean surface O3

The influence of ozone precursor emissions from four world regions on tropospheric composition and radiative climate forcing

Ozone (O-3) precursor emissions influence regional and global climate and air quality through changes in tropospheric O-3 and oxidants, which also influence methane (CH4) and sulfate aerosols (SO42-). We examine changes in the tropospheric composition of O-3, CH4, SO42- and global net radiative forcing (RF) for 20% reductions in global CH4 burden and in anthropogenic O-3 precursor emissions (NOx, NMVOC, and CO) from four regions (East Asia, Europe and Northern Africa, North America, and South Asia) using the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model (CTM) simulations, assessing uncertainty (mean +/- 1 standard deviation) across multiple CTMs. We evaluate steady state O-3 responses, including long-term feedbacks via CH4. With a radiative transfer model that includes greenhouse gases and the aerosol direct effect, we find that regional NOx reductions produce global, annually averaged positive net RFs (0.2 +/- 0.6 to 1.7 +/- 2 mWm(-2)/TgN yr(-1)), with some variation among models. Negative net RFs result from reductions in global CH4 (-162.6 +/- 2 mWm(-2) for a change from 1760 to 1408 ppbv CH4) and regional NMVOC (-0.4 +/- 0.2 to -0.7 +/- 0.2 mWm(-2)/Tg C yr(-1)) and CO emissions (-0.13 +/- 0.02 to -0.15 +/- 0.02 mWm(-2)/Tg CO yr(-1)). Including the effect of O-3 on CO2 uptake by vegetation likely makes these net RFs more negative by -1.9 to -5.2 mWm(-2)/Tg N yr(-1), -0.2 to -0.7 mWm(-2)/Tg C yr(-1), and -0.02 to -0.05 mWm(-2)/Tg CO yr(-1). Net RF impacts reflect the distribution of concentration changes, where RF is affected locally by changes in SO42-, regionally to hemispherically by O-3, and globally by CH4. Global annual average SO42- responses to oxidant changes range from 0.4 +/- 2.6 to -1.9 +/- 1.3 Gg for NOx reductions, 0.1 +/- 1.2 to -0.9 +/- 0.8 Gg for NMVOC reductions, and -0.09 +/- 0.5 to -0.9 +/- 0.8 Gg for CO reductions, suggesting additional research is needed. The 100-year global warming potentials (GWP(100)) are calculated for the global CH4 reduction (20.9 +/- 3.7 without stratospheric O-3 or water vapor, 24.2 +/- 4.2 including those components), and for the regional NOx, NMVOC, and CO reductions (-18.7 +/- 25.9 to -1.9 +/- 8.7 for NOx, 4.8 +/- 1.7 to 8.3 +/- 1.9 for NMVOC, and 1.5 +/- 0.4 to 1.7 +/- 0.5 for CO). Variation in GWP(100) for NOx, NMVOC, and CO suggests that regionally specific GWPs may be necessary and could support the inclusio