Evaluating global emission inventories of biogenic bromocarbons

  • 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 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) 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 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 West 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 (BryVSLS). Our simulations show BryVSLS 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) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.

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Author:Ryan Hossaini, Hannah Mantle, Martyn P. Chipperfield, Stephen A. Montzka, Paul Hamer, Franziska Ziska, Birgit Quack, Kirstin Krüger, Susann TegtmeierORCiDGND, Elliot L. Atlas, Stephan Sala, Andreas EngelORCiD, Harald Bönisch, Timo Keber, David Oram, Graham Mills, Carlos Ordóñez, Alfonso Saiz-Lopez, Nicola Warwick, Qing Liang, Wuhu Feng, Fred Moore, Benjamin R. Miller, Virginie Marécal, Nigel A. D. Richards, Marcel Klaus Dorf, Klaus Pfeilsticker
URN:urn:nbn:de:hebis:30:3-329089
DOI:https://doi.org/10.5194/acpd-13-12485-2013
ISSN:1680-7375
ISSN:1680-7367
Parent Title (English):Atmospheric chemistry and physics / Discussions, 13.2013, S. 12485-12539
Publisher:European Geosciences Union
Place of publication:Katlenburg-Lindau
Document Type:Article
Language:English
Date of Publication (online):2013/05/14
Date of first Publication:2013/05/14
Publishing Institution:Universitätsbibliothek Johann Christian Senckenberg
Release Date:2014/02/03
Volume:13
Page Number:55
First Page:12485
Last Page:12539
Note:
© Author(s) 2013. This work is distributed under the Creative Commons Attribution 3.0 License.
HeBIS-PPN:36372236X
Institutes:Geowissenschaften / Geographie / Geowissenschaften
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 55 Geowissenschaften, Geologie / 550 Geowissenschaften
Sammlungen:Universitätspublikationen
Licence (German):License LogoCreative Commons - Namensnennung 3.0