Measurements of bromine monoxide over four halogen activation seasons in the Canadian high Arctic

Abstract

<p><span>Bromine explosions and corresponding ozone depletion events (ODEs) are common in the Arctic spring. The snowpack on sea ice and sea salt aerosols (SSA) are both thought to release bromine, but the relative contribution of each source is not yet known. Furthermore, the role of atmospheric conditions is not fully understood. Long-term measurements of bromine monoxide (BrO) provide useful insight into the underlying processes of bromine activation. Here we present a four-year dataset (2016-2019) of springtime BrO partial columns retrieved from Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements in Eureka, Canada (80.1° N, 86.4° W). Due to the altitude of the measurement site (610 m), the measurements often represent BrO above the shallow boundary layer, and the strength of the temperature inversion has limited impact on the BrO partial columns. When the boundary layer is deep, however, the effects of the enhanced vertical mixing manifest as an increase in the minimum BrO values (and reduced ODE frequency) for wind speeds of ~8 m/s or greater. We find that BrO events show two modes differentiated by local wind direction and air mass history. Longer time spent in first-year sea ice areas corresponds to increased BrO for one of these modes only. We argue that snow on multi-year ice (salted and acidified by Arctic haze) might also contribute to bromine release. The MAX-DOAS measurements show that high aerosol optical depth is required to maintain lofted BrO. In situ measurements indicate that accumulation mode aerosols (mostly Arctic haze) have no direct correlation with BrO. The presence of coarse mode aerosols, however, is a necessary and sufficient condition for observing enhanced BrO at Eureka. The measurements of coarse mode aerosols are consistent with SSA generated from blowing snow. The good correlation between BrO and coarse mode aerosols (R<sup>2</sup> up to 0.57) supports the view that SSA is a direct source of bromine to the polar troposphere.</span></p>