Journal cover Journal topic
Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
doi:10.5194/acp-2016-1141
© Author(s) 2017. This work is distributed
under the Creative Commons Attribution 3.0 License.
Research article
23 Feb 2017
Review status
A revision of this discussion paper was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.
Observations of Bromine Monoxide Transport In the Arctic Sustained on Aerosol Particles
Peter K. Peterson1, Denis Pöhler2, Holger Sihler2,3, Johannes Zielcke2, Stephan General2, Udo Frieß2, Ulrich Platt2,3, William R. Simpson4, Son V. Nghiem5, Paul B. Shepson6, Brian H. Stirm7, Suresh Dhaniyala8, Thomas Wagner3, Dana R. Caulton9, Jose D. Fuentes10, and Kerri A. Pratt1,11 1Department of Chemistry, University of Michigan, Ann Arbor, MI, USA
2Institute of Environmental Physics, University of Heidelberg, Heidelberg, Germany
3Max Planck Institute for Chemistry, Mainz, Germany
4Department of Chemistry and Biochemistry and Geophysical Institute, University of Alaska Fairbanks, Fairbanks, Alaska, USA
5Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USA
6Department of Chemistry, Department of Earth, Planetary, and Atmospheric Sciences, and Purdue Climate Change Research Center, Purdue University, West Lafayette, IN, USA
7School of Aviation and Transportation Technology, Purdue University, West Lafayette, IN, USA
8Department of Mechanical and Aeronautical Engineering, Clarkson University, Potsdam, NY, USA
9Department of Civil and Environmental Engineering, Princeton University, Princeton, NJ, USA
10Department of Meteorology, The Pennsylvania State University, University Park, PA, USA
11Department of Earth and Environmental Sciences, University of Michigan, Ann Arbor, MI, USA
Abstract. 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.

Citation: Peterson, P. K., Pöhler, D., Sihler, H., Zielcke, J., General, S., Frieß, U., Platt, U., Simpson, W. R., Nghiem, S. V., Shepson, P. B., Stirm, B. H., Dhaniyala, S., Wagner, T., Caulton, D. R., Fuentes, J. D., and Pratt, K. A.: Observations of Bromine Monoxide Transport In the Arctic Sustained on Aerosol Particles, Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-1141, in review, 2017.
Peter K. Peterson et al.
Interactive discussionStatus: closed
AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment
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RC1: 'review of Peterson et al. paper', Anonymous Referee #1, 20 Mar 2017 Printer-friendly Version 
AC1: 'Response to Reviewer #1', Kerri Pratt, 18 May 2017 Printer-friendly Version Supplement 
 
RC2: 'Peterson et al. review', Anonymous Referee #2, 16 Apr 2017 Printer-friendly Version 
AC2: 'Response to Reviewer #2', Kerri Pratt, 18 May 2017 Printer-friendly Version Supplement 
Peter K. Peterson et al.
Peter K. Peterson et al.

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Short summary
High spatial resolution aircraft measurements in the Arctic showed the sustained transport of reactive bromine in a lofted layer via heterogeneous reactions on aerosol particles. This process provides a means to extend the spatial extent of the influence of halogen chemistry on atmospheric composition. The knowledge gained herein improves our ability to interpret satellite observations and simulate impacts of this chemistry on the fate and transport of atmospheric pollutants.
High spatial resolution aircraft measurements in the Arctic showed the sustained transport of...
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