The NASA TRACE A experiment (September – October 1992) investigated effects of dry season biomass burning emissions from both South America and southern Africa on the tropical South Atlantic troposphere. Whole air canister samples were collected aboard the NASA DC‐8 aircraft and analyzed for a wide range of nonmethane hydrocarbons (NMHCs) and halocarbons. Fast response in situ quantification of CH4, CO, and CO2 were also performed on the DC‐8. Sampling took place over Brazilian agricultural areas and southern African savanna where there was active biomass burning. The vertical distribution of the measured gases revealed that the concentrations of most hydrocarbons, methyl halides, CH4, CO, and CO2, were enhanced in the boundary layer of these regions principally as a result of biomass fires. Brazilian and African biomass burning emission ratios were calculated for CH3Br, CH3Cl, CH3I, and NMHCs relative to CO and CO2. Although both fire regions were dominated by efficient (flaming) combustion (CO/CO2 ratios <0.1), the Brazilian samples exhibited the lower (more flaming) CO/CO2 ratio of 0.037 compared with the African savanna value of 0.062. This difference in combustion efficiency was reflected in lower ratios versus CO2 for all correlated gases. However, the gases more closely associated with smoldering combustion (e.g., C3H8 and CH3Cl) exhibited significantly higher ratios relative to CO for the Brazilian fires, while the African samples exhibited higher values versus CO for compounds associated more closely with flaming combustion (e.g., C2H2). This variation in the trace gas ratios versus CO is most likely caused by different fuel characteristics. On the basis of the emission ratios obtained, the total biomass burning emission rates for savannas and worldwide were calculated for the hydrocarbons and methyl halides. From these it was estimated that roughly 25% and 20% of global CH3Cl and CH3Br emissions, respectively, derive from biomass burning but that the contribution of biomass burning to total CH3I emissions was not significant.

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A total of 1667 whole air samples were collected onboard the NASA DC-8 aircraft during the 6-week Pacific Exploratory Mission over the western Pacific (PEM-West A) in September and October 1991. The samples were assayed for 15 C2-C7 hydrocarbons and six halocarbons. Latitudinal (0.5øS to 59.5øN) and longitudinal (114øE to 122øW) profiles were obtained from samples collected between ground level and 12.7 km. Thirteen of the 18 missions exhibited at least one vertical profile where the hydrocarbon mixing ratios increased with altitude. Longitude-latitude color patch plots at three altitude levels and three-dimensional color latitudealtitude and longitude-altitude contour plots exhibit a significant number of middle-upper tropospheric pollution events. These and several lower tropospheric pollution plumes were characterized by comparison with urban data from Tokyo and Hong Kong, as well as with natural gas and the products from incomplete combustion. Elevated levels of nonmethane hydrocarbons (NMHC) and other trace gases in the upper-middle free troposphere were attributed to deep convection over the Asian continent and to typhoon-driven convection near the western Pacific coast of Asia. In addition, NMHCs and CH3CC13 were found to be useful tracers with which to distinguish hydrocarbon and halocarbon augmented plumes emiued from coastal Asian cities into the northwestern Pacific.

[1] Global measurements show that the mixing ratio of tropospheric methane (CH 4 ) increased by 1.1% (19.5 ± 1.7 ppbv) over the five-year period 1996 -2000, with striking fluctuations in its annual growth rate. Whereas the global CH 4 growth rate reached 15.9 ± 0.7 ppbv yr À1 in 1998, the growth rate was À2.1 ± 0.8 ppbv yr À1 in 2000. This is the first time in our 23-year global monitoring program that we have measured a negative annual CH 4 growth rate. The CH 4 growth rate fluctuates in an unpredictable fashion, and we reemphasize that global CH 4 concentrations cannot be extrapolated into the future based on past trends. As a result, we suggest that the slowing of the CH 4 growth rate during much of the 1980s and 1990s cannot be used to imply that CH 4 will no longer be of concern in greenhouse gas studies during this century.

Approximately 1000 whole air samples were collected and assayed for selected C2‐C5 hydrocarbons during the 6‐week Arctic Boundary Layer Expedition (ABLE 3A). Transit flights enabled latitudinal (40°N to 83°N) and longitudinal (70°W to 155°W) profiles to be obtained for altitudes between 4000 and 6000 m yielding summertime background mixing ratios for ethane, ethyne, propane and n‐butane of 1050±200, 100±40, 120±80 and 10±8 pptv, respectively. Drilling associated with oil exploration in the Alaskan North Slope area is suggested to be a probable source of the enhanced levels of alkanes observed in the Arctic region within a radius in excess of 300 km from Prudhoe Bay, Alaska. A significant number of pollution plumes were encountered which could be attributed to wildfires. Factors describing the emissions caused by biomass burning relative to ethane for ethyne (0.40) and propane (0.08) were determined. An increase of hydrocarbon mixing ratios with altitude was observed during all but two of the missions. Therefore, the Arctic and sub‐Arctic are significantly influenced by the long‐range transport of pollutants from nonlocal sources. A single vertical profile made in the vicinity of Wallops Island, Virginia, revealed elevated levels of isoprene, numerous hydrocarbons of the types associated with the leakage of natural gas and fossil fuel combustion, and substantial concentrations of nitrogen oxides and ozone. This implies that long‐range transport of various gases from urban areas, combined with local biogenic emissions of isoprene, are significant sources of regional tropospheric ozone.