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Abstract

Ozone depletion events (ODEs) are a common occurence 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 auto-catalytic 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 as well as 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 Utqiag ̇vik, 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 Nord Station, 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 TROPOMI observations. BrO VCDs above 5 × 1013 molec/cm2 observed by the satellite agree well with the model results. However, the model also predicts BrO VCDs of around 3 × 1013 molec/cm2 throughout the Arctic and patches of BrO VCDs of around 1014 molec/cm2 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.