Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 6 6 2006 10.5194/acpd-6-11465-2006 http://www.atmos-chem-phys-discuss.net/6/11465/2006/ http://www.atmos-chem-phys-discuss.net/6/11465/2006/acpd-6-11465-2006.html http://www.atmos-chem-phys-discuss.net/6/11465/2006/acpd-6-11465-2006.pdf 11465 11520 2006-11-17 Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone B. Sauvage R. V. Martin A. van Donkelaar X. Liu K. Chance L. Jaeglé P. I. Palmer S. Wu T.-M. Fu Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia, Canada Atomic and Molecular Physics Division, Harvard-Smithsonian Center for Astrophysics, Cambridge, Massachusetts, USA Department of Atmospheric Sciences, University of Washington, Seattle, Washington, USA School of GeoSciences, University of Edinburgh, UK Department of Earth and Planetary Sciences and Division of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O₃, NO₂, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O₃, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O₃ from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O₃ in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O₃ columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO₂ and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NO_x (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NO_x over northern equatorial Africa. These emissions increase lower tropospheric O₃ by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O₃ columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O₃ observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO₃ on aerosols reduces simulated O₃ by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO₂ uptake on aerosols improves O₃ by 5 ppbv in biomass burning regions.