Abstract. Halogenated very short-lived substances (VSLSs), such as bromoform
(CHBr3), can be transported to the stratosphere and contribute to the
halogen loading and ozone depletion. Given their highly variable emission
rates and their short atmospheric lifetimes, the exact amount as well as the
spatio-temporal variability of their contribution to the stratospheric halogen
loading are still uncertain. We combine observational data sets with
Lagrangian atmospheric modelling in order to analyse the spatial and
temporal variability of the CHBr3 injection into the stratosphere for
the time period 1979–2013. Regional maxima with mixing ratios of up to
0.4–0.5 ppt at 17 km 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 timescales 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 aircraft measurements during the ACCENT
campaign and do not occur in spatially or temporally averaged model fields.
CHBr3 injection over the west Pacific is centred south of the Equator
due to strong oceanic sources underneath prescribed by the here-applied
bottom-up emission inventory. The globally largest CHBr3 mixing ratios
at the cold point level of up to 0.6 ppt are 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. Inter-annual
variability of stratospheric CHBr3 injection of 10 %–20 % 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
sea surface temperature 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±0.012 ppt Br per decade for 1979–2013, corresponding to 3 % Br per decade. The overall contribution of CHBr3 together with
CH2Br2 to the stratospheric halogen loading accounts for 4.7 ppt Br, in good agreement with existing studies, with 50 % and 50 % being
injected in the form of source and product gases, respectively.