TY  - JOUR
A1  - Hossaini, Ryan
A1  - Mantle, Hannah
A1  - Chipperfield, Martyn P.
A1  - Montzka, Stephen A.
A1  - Hamer, Paul
A1  - Ziska, Franziska
A1  - Quack, Birgit
A1  - Krüger, Kirstin
A1  - Tegtmeier, Susann
A1  - Atlas, Elliot L.
A1  - Sala, Stephan
A1  - Engel, Andreas
A1  - Bönisch, Harald
A1  - Keber, Timo
A1  - Oram, David
A1  - Mills, Graham
A1  - Ordóñez, Carlos
A1  - Saiz-Lopez, Alfonso
A1  - Warwick, Nicola
A1  - Liang, Qing
A1  - Feng, Wuhu
A1  - Moore, Fred
A1  - Miller, Benjamin R.
A1  - Marécal, Virginie
A1  - Richards, Nigel A. D.
A1  - Dorf, Marcel Klaus
A1  - Pfeilsticker, Klaus
T1  - Evaluating global emission inventories of biogenic bromocarbons
T2  - Atmospheric chemistry and physics
N2  - 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 oxidising 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 (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 (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.
Y1  - 2013
UR  - http://publikationen.ub.uni-frankfurt.de/frontdoor/index/index/docId/32909
UR  - https://nbn-resolving.org/urn:nbn:de:hebis:30:3-329099
SN  - 1680-7324
N1  - © Author(s) 2013. This work is distributed under the Creative Commons Attribution 3.0 License.
VL  - 13
SP  - 11819
EP  - 11838
PB  - European Geosciences Union
CY  - Katlenburg-Lindau
ER  -