Photochemical smog, or ground-level ozone, has been the most recalcitrant of air pollution problems, but reductions in emissions of sulfur and hydrocarbons may yield unanticipated benefits in air quality. While sulfate and some organic aerosol particles scatter solar radiation back into space and can cool Earth's surface, they also change the actinic flux of ultraviolet (UV) radiation. Observations and numerical models show that UV-scattering particles in the boundary layer accelerate photochemical reactions and smog production, but UV-absorbing aerosols such as mineral dust and soot inhibit smog production. Results could have major implications for the control of air pollution.

[1] Smoke and pollutants from Canadian forest fires are sometimes transported over the United States at low altitudes behind advancing cold fronts. An unusual event occurred in July 2002 in which smoke from fires in Quebec was observed by satellite, lidar, and aircraft to arrive over the Washington, D.C., area at high altitudes. This elevated smoke plume subsequently mixed to the surface as it was entrained into the turbulent planetary boundary layer and had adverse effects on the surface air quality over the region. Trajectory and three-dimensional model calculations confirmed the origin of the smoke, its transport at high altitudes, and the mechanism for bringing the pollutants to the surface. Additionally, the modeled smoke optical properties agreed well with aircraft and remote sensing observations provided the smoke particles were allowed to age by coagulation in the model. These results have important implications for the long-range transport of pollutants and their subsequent entrainment to the surface, as well as the evolving optical properties of smoke from boreal forest fires.

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Observations at sites in eastern North America show a strong correlation between O3 and CO concentrations in summer, with a consistent slope ΔO3/ΔCO ≈ 0.3. Observations in the aged Denver plume at Niwot Ridge, Colorado, also show a strong correlation but with ΔO3/ΔCO = 0.15. These data offer a sensitive test for evaluating the ability of photochemical models to simulate production of O3 over North America and its export to the global atmosphere. Application to the Harvard/Goddard Institute for Space Studies three‐dimensional, continental‐scale model shows that the model gives a good simulation of the observed O3‐CO correlations and of the associated ΔO3/ΔCO. This successful simulation lends support to model estimates of 6 Gmol d−1 for the net O3 production in the U.S. boundary layer in summer (corresponding to a net O3 production efficiency of 5.5, which is the number of O3 molecules produced per molecule of NOx consumed) and 70% for the fraction of the net production that is exported to the global atmosphere. Export of U.S. pollution appears to make a significant contribution to total tropospheric O3 over the northern hemisphere in summer. Simple interpretation of observed ΔO3/ΔCO as an O3/CO anthropogenic enhancement ratio is shown to underestimate substantially anthropogenic O3 production, because O3 and CO concentrations are negatively correlated in the absence of photochemistry. It is also shown that concurrent observations of ΔO3/ΔCO and ΔO3/Δ(NOy‐NOx) ratios can be used to impose lower and upper limits on the net O3 production efficiency.