Popis: |
The return of sunlight in the polar spring leads to production of reactive halogen species from the surface snowpack, significantly altering the chemical composition of the Arctic near-surface atmosphere and the fate of long-range transported pollutants, including mercury. Recent work has shown the initial production of reactive bromine at the Arctic surface snowpack; however, we have limited knowledge of the vertical extent of this chemistry, as well as the lifetime and possible transport of reactive bromine aloft. Here, we present bromine monoxide (BrO) and aerosol particle measurements obtained during the March 2012 BRomine Ozone Mercury EXperiment (BROMEX) near Utqiagvik (Barrow), AK. The airborne differential optical absorption spectroscopy (DOAS) measurements provided an unprecedented level of spatial resolution, over two orders of magnitude greater than satellite observations and with vertical resolution unable to be achieved by satellite methods, for BrO in the Arctic. This novel method provided quantitative identification of a BrO plume, disconnected from the surface, moving at the speed of the air mass. This lofted reactive bromine plume was transported and maintained at elevated levels through heterogeneous reactions on co-located supermicron aerosol particles, independently of surface snowpack bromine chemistry. This chemical transport mechanism significantly increases the spatial extent of this reactive bromine chemistry, impacting atmospheric composition and pollutant fate across the region, beyond the area of initial snowpack halogen production. This process must be considered in the interpretation of satellite BrO observations and examined in the context of the rapidly changing Arctic sea ice and snowpack. |