Evaluating global emission inventories of biogenic bromocarbons

Hossaini, R. and Mantle, H. and Chipperfield, M. P. and Montzka, S. A. and Hamer, P. and Ziska, E. and Quack, B. and Krueger, K. and Tegtmeier, S. and Atlas, E. and Sala, S. and Engel, A. and Boenisch, H. and Keber, T. and Oram, D. and Mills, G. and Ordonez, C. and Saiz-Lopez, A. and Warwick, N. and Liang, Q. and Feng, W. and Moore, E. and Miller, B. R. and Marecal, V. and Richards, N. A. D. and Dorf, M. and Pfeilsticker, K. (2013) Evaluating global emission inventories of biogenic bromocarbons. Atmospheric Chemistry and Physics, 13 (23). pp. 11819-11838. ISSN 1680-7316

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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 (Br-y) loading in both the troposphere, where bromine chemistry perturbs global oxidising capacity, and in the stratosphere, where it is a major sink for ozone (O-3). We have performed simulations using a 3-D chemical transport model (CTM) including three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform (CHBr3) and dibromomethane (CH2Br2). We perform the first concerted evaluation of these inventories, comparing both the magnitude and spatial distribution of emissions. For a quantitative evaluation of each inventory, model output is compared with independent long-term observations at National Oceanic and Atmospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF (National Science Foundation) HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 (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 aircraft observations made during the 2011 Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere (SHIVA) campaign, in the tropical western Pacific. Here, the performance of the various inventories also varies significantly, but overall the CTM is able 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 (Br-y(VSLS)). Our simulations show Br-y(VSLS) ranges from similar to 4.0 to 8.0 ppt depending on the inventory. We report an optimised estimate at the lower end of this range (similar to 4 ppt) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.

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Journal Article
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Atmospheric Chemistry and Physics
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24 Oct 2016 10:02
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19 Sep 2023 01:36