Surface fluxes of bromoform and dibromomethane over the tropical western Pacific inferred from airborne in situ measurements
2017
Abstract. We infer surface fluxes of bromoform ( CHBr 3 ) and
dibromoform ( CH 2 Br 2 ) from aircraft observations over the western
Pacific using a tagged version of the GEOS-Chem global 3-D atmospheric
chemistry model and a maximum a posteriori inverse model. Using GEOS-Chem (GC) as
an intermediary, we find that the distribution of a priori ocean
emissions of these gases are reasonably consistent with observed atmospheric
mole fractions of CHBr 3 ( r =0.62 ) and CH 2 Br 2
( r =0.38 ). These a priori emissions result in a positive model bias
in CHBr 3 peaking in the marine boundary layer, but reproduce
observed values of CH 2 Br 2 with no significant bias by virtue of
its longer atmospheric lifetime. Using GEOS-Chem, we find that observed
variations in atmospheric CHBr 3 are determined equally by sources
over the western Pacific and those outside the study region, but observed
variations in CH 2 Br 2 are determined mainly by sources outside
the western Pacific. Numerical closed-loop experiments show that the spatial
and temporal distribution of boundary layer aircraft data have the potential
to substantially improve current knowledge of these fluxes, with improvements
related to data density. Using the aircraft data, we estimate aggregated
regional fluxes of 3.6 ± 0.3 × 10 8 and 0.7 ± 0.1 × 10 8 g month −1 for CHBr 3 and CH 2 Br 2 over
130–155 ∘ E and 0–12 ∘ N, respectively, which represent
reductions of 20 %–40 % of the prior inventories by Ordonez
et al. (2012) and substantial spatial deviations from different a
priori inventories. We find no evidence to support a robust linear
relationship between CHBr 3 and CH 2 Br 2 oceanic
emissions, as used by previous studies. We find that over regions with dense
observation coverage, our choice of a priori inventory does not
significantly impact our reported a posteriori flux estimates.
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