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Evaluating global emission inventories of biogenic bromocarbons

Hossaini R, Mantle H, Chipperfield M, Montzka S, Hamer P, Ziska F, Quack B, Krüger K, Tegtmeier S, Atlas E, Sala S, Engel A, Bönisch H, Keber T, Oram D, Mills G, Ordóñez C, Saiz-Lopez A, Warwick N, Liang Q, Feng W, Moore F, Miller B, Marécal V, Richards N, Dorf M, Pfeilsticker K ...see all

Atmospheric Chemistry and Physics, vol. 13, issue 23 (2013) pp. 11819-11838

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Abstract

Emissions of halogenated very short-lived substances (VSLS) are poorly constrained. However, their inclusion in global models is required to simulate a realistic inorganic bromine (Bry) loading in both the troposphere, where bromine chemistry perturbs 5 global oxidizing capacity, and in the stratosphere, where it is a major sink for ozone (O3). We have performed simulations using a 3-D chemical transport model (CTM) in- cluding three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform(CHBr3) and dibromomethane (CH2Br2).We performthe first concerted evaluation of these inventories, comparing both the magnitude and spa- 10 tial distribution of emissions. For a quantitative evaluation of each inventory, model out- put is compared with independent long-term observations at National Oceanic and At- mospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 15 (38%) to 0.78 (115%) parts per trillion (ppt) in the tropics, depending on emission inventory. For CH2Br2, the range is 0.17 (24%) to 1.25 (167%)ppt. We also use air- craft observations made during the 2011 “Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere” (SHIVA) campaign, in the tropicalWest Pacific. Here, the perfor- mance of the various inventories also varies significantly, but overall the CTM is able 20 to reproduce observed CHBr3 well in the free troposphere using an inventory based on observed sea-to-air fluxes. Finally, we identify the range of uncertainty associated with these VSLS emission inventories on stratospheric bromine loading due to VSLS (BrVSLS y ). Our simulations show BrVSLS y ranges from ∼4.0 to 8.0 ppt depending on the inventory. We report an optimised estimate at the lower end of this range (∼4 ppt) 25 based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics

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