Variability and long-term changes of brominated VSLS at the tropical tropopause

Abstract

Abstract. We combine available observational data sets with Lagrangian atmospheric modelling in order to analyze the spatial and temporal variability of the CHBr3 injection into the stratosphere. Regional maxima with mixing ratios of up to 0.4–0.5\u2009ppt at 17\u2009km altitude are diagnosed to be over Central America (1) and over the Maritime Continent/West Pacific (2), both of which are confirmed by high-altitude aircraft campaigns. The CHBr3 maximum over Central America is caused by the co-occurrence of convectively-driven short transport time scales and strong regional sources, which in conjunction drive the seasonality of CHBr3 injection. Model results at a daily resolution reveal isolated, exceptionally high CHBr3 values in this region which are confirmed by measurements during the ACCENT campaign and do not occur in spatially or temporally averaged model fields. CHBr3 injection over the West Pacific is centered south of the equator due to strong oceanic sources underneath prescribed by the here applied bottom-up emission inventory. The globally strongest stratospheric CHBr3 injection of up to 0.6\u2009ppt is diagnosed to occur over the region of India, Bay of Bengal and Arabian Sea (3), however, no data from aircraft campaigns are available to confirm this finding. Interannual variability of stratospheric CHBr3 injection of 10–20\u2009% is to a large part driven by the variability of coupled ocean-atmosphere circulation systems. Long-term changes, on the other hand, correlate with the regional SST trends resulting in positive trends of stratospheric CHBr3 injection over the West Pacific and Asian monsoon region and negative trends over the East Pacific. For the tropical mean, these opposite regional trends balance each other out resulting in a relatively weak positive trend of 0.017\u2009±\u20090.012\u2009ppt Br/dec for 1979–2013, corresponding 3\u2009% Br/dec. The overall contribution of CHBr3 together with CH2Br2 to the stratospheric halogen loading accounts for 4.7\u2009ppt Br, in good agreement with existing studies, with 50\u2009%/50\u2009% being injected in form of source and product gases, respectively.