アイテム詳細

要旨

Ozone depletion events (ODEs) are a common occurrence in the boundary layer during Arctic
spring. Ozone is depleted by bromine species, which are most likely emitted from snow, sea ice, or aerosols
in an autocatalytic reaction cycle. Previous three-dimensional modeling studies of ODEs assumed an infinite
bromine source at the ground. In the present study, an alternative emission scheme is presented in which a
finite amount of bromide in the snow is tracked over time. For this purpose, a modified version of the Weather
Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to study ODEs in the Arctic
from February to May 2019. The model data are compared to in situ measurements, ozone sonde flights, and
satellite data. A simulation of the ODEs in the Arctic spring of 2009 using the infinite-bromide assumption on
first-year (FY) ice is transferred to the spring of 2019, which achieves good agreement with the observations;
however, there is some disagreement in April 2009 and 2019 with respect to an overestimation concerning
both the magnitude and the number of ODEs. New simulations using the finite-bromide assumption greatly
improve agreement with in situ observations at Utqia ̇gvik, Alaska, Zeppelin Mountain, Svalbard, and Pallas,
Finland, in April 2019, suggesting that bromide on the sea ice is depleted to an extent that reduces the bromine
release. The new simulations also slightly improve the agreement with observations at these sites in February
and March. A comparison to measurements near Eureka, Canada, and Station Nord, Greenland, shows that
multi-year ice and possibly snow-covered land may be significant bromine sources. However, assuming higher
releasable bromide near Eureka does not remove all disagreement with the observations. The numerical results
are also compared to tropospheric-BrO vertical column densities generated with a new retrieval method from
TROPOspheric Monitoring Instrument (TROPOMI) observations. BrO vertical column densities (VCDs) above
5 × 1013 molec. cm−2 observed by the satellite agree well with the model results. However, the model also
predicts BrO VCDs of around 3 × 1013 molec. cm−2 throughout the Arctic and patches of BrO VCDs of around
1014 molec. cm−2 not observed by the satellite, especially near Hudson Bay. This suggests that snow at Hudson
Bay may be a weaker bromine source in late spring compared to snow in the north.