Acid deposition and photochemical smog are urban air pollution problems, and they remain localized as long as the sulfur, nitrogen, and hydrocarbon pollutants are confined to the lower troposphere (below about 1-kilometer altitude) where they are short-lived. If, however, the contaminants are rapidly transported to the upper troposphere, then their atmospheric residence times grow and their range of influence expands dramatically. Although this vertical transport ameliorates some of the effects of acid rain by diluting atmospheric acids, it exacerbates global tropospheric ozone production by redistributing the necessary nitrogen catalysts. Results of recent computer simulations suggest that thunderstorms are one means of rapid vertical transport. To test this hypothesis, several research aircraft near a midwestern thunderstrom measured carbon monoxide, hydrocarbons, ozone, and reactive nitrogen compounds. Their concentrations were much greater in the outflow region of the storm, up to 11 kilometers in altitude, than in surrounding air. Trace gas measurements can thus be used to track the motion of air in and around a cloud. Thunderstorms may transform local air pollution problems into regional or global atmospheric chemistry problems.
Measurements of H2O2 and related species were made by aircraft on 18 flights over 11 days during June 1987 over Ohio. Measurements typically encompassed an altitude range from the surface to 5.5 km above mean sea level and were conducted under a variety of meteorological conditions, but focussed on conditions conducive to the formation of convective storms. Concentrations of H2O2 ranged from <0.2 to 7 ppb and exhibited as much as a factor of 10 variability even on a given day at fixed altitude, as well as between days. Hydrogen peroxide concentration typically was low near the surface, rose to a maximum near the top of the boundary layer, then slowly decreased with altitude. In contrast, SO2 and NOy were largely confined to the surface layer. A simple photochemical calculation shows that where NOx concentrations are low, [H2O2] is strongly influenced by the water vapor concentration. The [H2O2] tracked changes in dew point, and measured and calculated H2O2 concentrations were in general agreement. The low [H2O2] in the boundary layer is ascribed to consumption of radicals by reactions other than combination reactions, and to loss of H2O2 by dry deposition. Comparison of the profile shapes for H2O2 and SO2 suggests that mixing processes will have a large influence on the extent to which these two species will react in convective systems.
The phase I Gametag (Global Atmospheric Measurements Experiment of Tropospheric Aerosols and Gases) aerosol measurements were designed to provide an initial assessment of the levels, types, and optical effects of tropospheric aerosols in remote marine and continental regions and to examine the possible causal relationships between the observed distributions and the dominant factors controlling aerosol population: chemical and physical transformations, source and sink strengths, and transport. We used size‐number data to determine mass concentrations and to estimate extinction, using nominal optical properties. Filter and impactor data have been used to determine aerosol composition, and correlative aircraft measurements have been used to aid in our data interpretation. Our data have been used to generate latitudinal profiles along our Pacific flight tracks. Our continental measurements, in general, show bimodal aerosol size distributions that reflect different source for each mode. The aerosol population consists primarily of crustal aerosols with r ≥ 0.5 μm and sulfate and combustion aerosols with r < 0.5 μm, with only a minor sea salt component. Owing to vertical mixing, there are no qualitative differences between the boundary layer and the free troposphere. Our data indicate that crustal aerosols represent a significant component of a background tropospheric aerosol in western North America and suggest that the possible contribution of the crustal aerosol to extinction should not be ignored. Pacific marine measurements show a qualitative difference between the boundary layer and the free troposphere. The boundary‐layer aerosol population is dominated by a bimodal sea spray aerosol; optical effects and mass concentration are dominated by a mode with a volume mean radius of ∼1 μm. Our measurements show only a small crustal component of the marine boundary‐layer aerosol. Our data indicate a loss of Cl from the sea spray aerosol, with the greatest loss in the small particles. We have inferred a background concentration of 0.2 ppbm for our measured particles that does not appear to be directly related to the sea spray aerosol. We have identified some of these particles as locally produced secondary aerosols; simultaneous measurements of gaseous species support this interpretation. Our Pacific free tropospheric aerosol measurements show a highly variable aerosol component, with local variations in concentration by 1 order of magnitude within a few kilometers. Our measured total aerosol and crustal component concentrations show a general decrease from north to south. Our lowest mean mid tropospheric concentration was seen south of 20°S; we have identified this mean concentration of 0.08 ppbm as a midtropospheric background aerosol.
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