Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - The contribution of natural and anthropogenic very short-lived species to stratospheric bromine
AU - Hossaini, R.
AU - Chipperfield, M. P.
AU - Feng, W.
AU - Breider, T. J.
AU - Atlas, E.
AU - Montzka, S. A.
AU - Miller, B. R.
AU - Moore, F.
AU - Elkins, J.
PY - 2012/1/5
Y1 - 2012/1/5
N2 - We have used a global three-dimensional chemical transport model to quantify the impact of the very short-lived substances (VSLS) CHBr3, CH2Br2, CHBr2Cl, CHBrCl2, CH2BrCl and C2H5Br on the bromine budget of the stratosphere. Atmospheric observations of these gases allow constraints on surface mixing ratios that, when incorporated into our model, contribute similar to 4.9-5.2 parts per trillion (ppt) of inorganic bromine (Br-y) to the stratosphere. Of this total, similar to 76% comes from naturally-emitted CHBr3 and CH2Br2. The remaining species individually contribute modest amounts. However, their accumulated total accounts for up to similar to 1.2 ppt of the supply and thus should not be ignored. We have compared modelled tropical profiles of a range of VSLS with observations from the recent 2009 NSF HIPPO-1 aircraft campaign. Modelled profiles agree reasonably well with observations from the surface to the lower tropical tropopause layer.We have also considered the poorly studied anthropogenic VSLS, C2H5Br, CH2BrCH2Br, n-C3H7Br and i-C3H7Br. We find the local atmospheric lifetime of these species in the tropical tropopause layer are similar to 183, 603, 39 and 49 days, respectively. These species, particularly C2H5Br and CH2BrCH2Br, would thus be important carriers of bromine to the stratosphere if emissions were to increase substantially. Our model shows similar to 70-73% and similar to 80-85% of bromine from these species in the tropical boundary layer can reach the lower stratosphere.
AB - We have used a global three-dimensional chemical transport model to quantify the impact of the very short-lived substances (VSLS) CHBr3, CH2Br2, CHBr2Cl, CHBrCl2, CH2BrCl and C2H5Br on the bromine budget of the stratosphere. Atmospheric observations of these gases allow constraints on surface mixing ratios that, when incorporated into our model, contribute similar to 4.9-5.2 parts per trillion (ppt) of inorganic bromine (Br-y) to the stratosphere. Of this total, similar to 76% comes from naturally-emitted CHBr3 and CH2Br2. The remaining species individually contribute modest amounts. However, their accumulated total accounts for up to similar to 1.2 ppt of the supply and thus should not be ignored. We have compared modelled tropical profiles of a range of VSLS with observations from the recent 2009 NSF HIPPO-1 aircraft campaign. Modelled profiles agree reasonably well with observations from the surface to the lower tropical tropopause layer.We have also considered the poorly studied anthropogenic VSLS, C2H5Br, CH2BrCH2Br, n-C3H7Br and i-C3H7Br. We find the local atmospheric lifetime of these species in the tropical tropopause layer are similar to 183, 603, 39 and 49 days, respectively. These species, particularly C2H5Br and CH2BrCH2Br, would thus be important carriers of bromine to the stratosphere if emissions were to increase substantially. Our model shows similar to 70-73% and similar to 80-85% of bromine from these species in the tropical boundary layer can reach the lower stratosphere.
KW - CHEMICAL-TRANSPORT MODEL
KW - UPPER TROPOSPHERE
KW - TRACER TRANSPORT
KW - DEEP CONVECTION
KW - BR-Y
KW - VALIDATION
KW - SUBSTANCES
KW - BROMOFORM
KW - SCHEMES
KW - TROPICS
U2 - 10.5194/acp-12-371-2012
DO - 10.5194/acp-12-371-2012
M3 - Journal article
VL - 12
SP - 371
EP - 380
JO - Atmospheric Chemistry and Physics
JF - Atmospheric Chemistry and Physics
SN - 1680-7316
IS - 1
ER -