We use space-based observations of NO2 columns from the Global Ozone Monitoring Experiment (GOME) to derive monthly top-down NOx emissions for 2000 via inverse modeling with the GEOS-CHEM chemical transport model. Top-down NOx sources are partitioned among fuel combustion (fossil fuel and biofuel), biomass burning and soils by exploiting the spatio-temporal distribution of remotely sensed fires and a priori information on the location of regions dominated by fuel combustion. The top-down inventory is combined with an a priori inventory to obtain an optimized a posteriori estimate of the relative roles of NOx sources. The resulting a posteriori fuel combustion inventory (25.6 TgN year(-1)) agrees closely with the a priori (25.4 TgN year(-1)), and errors are reduced by a factor of 2, from +/- 80% to +/- 40%. Regionally, the largest differences are found over Japan and South Africa, where a posteriori estimates are 25% larger than a priori. A posteriori fuel combustion emissions are aseasonal, with the exception of East Asia and Europe where winter emissions are 30-40% larger relative to summer emissions, consistent with increased energy use during winter for heating. Global a posteriori biomass burning emissions in 2000 resulted in 5.8 TgN (compared to 5.9 TgN year(-1) in the a priori), with Africa accounting for half of this total. A posteriori biomass burning emissions over Southeast Asia/India are decreased by 46% relative to a priori; but over North equatorial Africa they are increased by 50%. A posteriori estimates of soil emissions (8.9 TgN year(-1)) are 68% larger than a priori (5.3 TgN year(-1)). The a posteriori inventory displays the largest soil emissions over tropical savanna/woodland ecosystems (Africa), as well as over agricultural regions in the western U.S. (Great Plains), southern Europe (Spain, Greece, Turkey), and Asia (North China Plain and North India), consistent with field measurements. Emissions over these regions are highest during summer at mid-latitudes and during the rainy season in the Tropics. We estimate that 2.5-4.5 TgN year(-1) are emitted from N-fertilized soils, at the upper end of previous estimates. Soil and biomass burning emissions account for 22% and 14% of global surface NOx emissions, respectively. We infer a significant role for soil NOx emissions at northern mid-latitudes during summer, where they account for nearly half that of the fuel combustion source, a doubling relative to the a priori. The contribution of soil emissions to background ozone is thus likely to be underestimated by the current generation of chemical transport models.

[1] We use space-based observations of NO 2 columns from the Global Ozone Monitoring Experiment (GOME) to map the spatial and seasonal variations of NO x emissions over Africa during 2000. The GOME observations show not only enhanced tropospheric NO 2 columns from biomass burning during the dry season but also comparable enhancements from soil emissions during the rainy season over the Sahel. These soil emissions occur in strong pulses lasting 1-3 weeks following the onset of rain, and affect 3 million km 2 of semiarid sub-Saharan savanna. Surface observations of NO 2 from the International Global Atmospheric Chemistry (IGAC)/Deposition of Biochemically Important Trace Species (DEBITS)/Africa (IDAF) network over West Africa provide further evidence for a strong role for microbial soil sources. By combining inverse modeling of GOME NO 2 columns with space-based observations of fires, we estimate that soils contribute 3.3 ± 1.8 TgN/year, similar to the biomass burning source (3.8 ± 2.1 TgN/year), and thus account for 40% of surface NO x emissions over Africa. Extrapolating to all the tropics, we estimate a 7.3 TgN/year biogenic soil source, which is a factor of 2 larger compared to model-based inventories but agrees with observationbased inventories. These large soil NO x emissions are likely to significantly contribute to the ozone enhancement originating from tropical Africa.

[1] The processes that determine which areas are strong sources of mineral aerosols are not well known. In this study we consider the role of ephemeral lakes in modulating emissions of atmospheric mineral aerosols. We focus on two ephemeral lake regions that have been identified as source regions: the zone of Chotts in Tunisia and Algeria, and Etosha Pan in Namibia. Comparisons of satellite retrieved inundation data and the TOMS absorbing aerosol index suggest that during some periods of inundation, desert dust loadings are reduced. There is some indication that after flooded areas have dried there is increased dust loading. However, the role of the inundated ephemeral lake compared with nearby regions in modulating desert dust sources is unclear, in addition, problems with interpreting the TOMS AI make conclusions difficult. More research is required to understand the small-scale sources of atmospheric desert dust in dry, unvegetated, topographic lows.