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| Titel |
Evaluating global emission inventories of biogenic bromocarbons |
| VerfasserIn |
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marecal, N. A. D. Richards, M. Dorf, K. Pfeilsticker |
| Medientyp |
Artikel
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| Sprache |
Englisch
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| ISSN |
1680-7316
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| Digitales Dokument |
URL |
| Erschienen |
In: Atmospheric Chemistry and Physics ; 13, no. 23 ; Nr. 13, no. 23 (2013-12-06), S.11819-11838 |
| Datensatznummer |
250085858
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| Publikation (Nr.) |
 copernicus.org/acp-13-11819-2013.pdf |
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| Zusammenfassung |
| 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. |
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