Observations of bromine monoxide transport in the Arctic sustained on aerosol particles

The return of sunlight in the polar spring leads to the 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 sho...

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Main Authors: P. K. Peterson, D. Pöhler, H. Sihler, J. Zielcke, S. General, U. Frieß, U. Platt, W. R. Simpson, S. V. Nghiem, P. B. Shepson, B. H. Stirm, S. Dhaniyala, T. Wagner, D. R. Caulton, J. D. Fuentes, K. A. Pratt
Format: Article
Language:English
Published: Copernicus Publications 2017-06-01
Series:Atmospheric Chemistry and Physics
Online Access:http://www.atmos-chem-phys.net/17/7567/2017/acp-17-7567-2017.pdf
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author P. K. Peterson
D. Pöhler
H. Sihler
H. Sihler
J. Zielcke
S. General
U. Frieß
U. Platt
U. Platt
W. R. Simpson
S. V. Nghiem
P. B. Shepson
B. H. Stirm
S. Dhaniyala
T. Wagner
D. R. Caulton
J. D. Fuentes
K. A. Pratt
K. A. Pratt
author_facet P. K. Peterson
D. Pöhler
H. Sihler
H. Sihler
J. Zielcke
S. General
U. Frieß
U. Platt
U. Platt
W. R. Simpson
S. V. Nghiem
P. B. Shepson
B. H. Stirm
S. Dhaniyala
T. Wagner
D. R. Caulton
J. D. Fuentes
K. A. Pratt
K. A. Pratt
author_sort P. K. Peterson
collection DOAJ
description The return of sunlight in the polar spring leads to the 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 Utqiaġvik (Barrow), AK. The airborne differential optical absorption spectroscopy (DOAS) measurements provided an unprecedented level of spatial resolution, over 2 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, between 500 m and 1 km aloft, moving at the speed of the air mass. Concurrent aerosol particle measurements suggest that this lofted reactive bromine plume was transported and maintained at elevated levels through heterogeneous reactions on colocated supermicron aerosol particles, independent of surface snowpack bromine chemistry. This chemical transport mechanism explains the large spatial extents often observed for reactive bromine chemistry, which impacts atmospheric composition and pollutant fate across the Arctic region, beyond areas of initial snowpack halogen production. The possibility of BrO enhancements disconnected from the surface potentially contributes to sustaining BrO in the free troposphere and must also be considered in the interpretation of satellite BrO column observations, particularly in the context of the rapidly changing Arctic sea ice and snowpack.
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spelling doaj.art-0fa9b84eda1d443ba8848bd7dc9cf1922022-12-21T19:39:38ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242017-06-01177567757910.5194/acp-17-7567-2017Observations of bromine monoxide transport in the Arctic sustained on aerosol particlesP. K. Peterson0D. Pöhler1H. Sihler2H. Sihler3J. Zielcke4S. General5U. Frieß6U. Platt7U. Platt8W. R. Simpson9S. V. Nghiem10P. B. Shepson11B. H. Stirm12S. Dhaniyala13T. Wagner14D. R. Caulton15J. D. Fuentes16K. A. Pratt17K. A. Pratt18Department of Chemistry, University of Michigan, Ann Arbor, MI, USAInstitute of Environmental Physics, University of Heidelberg, Heidelberg, GermanyInstitute of Environmental Physics, University of Heidelberg, Heidelberg, GermanyMax Planck Institute for Chemistry, Mainz, GermanyInstitute of Environmental Physics, University of Heidelberg, Heidelberg, GermanyInstitute of Environmental Physics, University of Heidelberg, Heidelberg, GermanyInstitute of Environmental Physics, University of Heidelberg, Heidelberg, GermanyInstitute of Environmental Physics, University of Heidelberg, Heidelberg, GermanyMax Planck Institute for Chemistry, Mainz, GermanyDepartment of Chemistry and Biochemistry and Geophysical Institute, University of Alaska Fairbanks, Fairbanks, Alaska, USAJet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USADepartment of Chemistry, Department of Earth, Planetary, and Atmospheric Sciences, and Purdue Climate Change Research Center, Purdue University, West Lafayette, IN, USASchool of Aviation and Transportation Technology, Purdue University, West Lafayette, IN, USADepartment of Mechanical and Aeronautical Engineering, Clarkson University, Potsdam, NY, USAMax Planck Institute for Chemistry, Mainz, GermanyDepartment of Civil and Environmental Engineering, Princeton University, Princeton, NJ, USADepartment of Meteorology, The Pennsylvania State University, University Park, PA, USADepartment of Chemistry, University of Michigan, Ann Arbor, MI, USADepartment of Earth and Environmental Sciences, University of Michigan, Ann Arbor, MI, USAThe return of sunlight in the polar spring leads to the 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 Utqiaġvik (Barrow), AK. The airborne differential optical absorption spectroscopy (DOAS) measurements provided an unprecedented level of spatial resolution, over 2 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, between 500 m and 1 km aloft, moving at the speed of the air mass. Concurrent aerosol particle measurements suggest that this lofted reactive bromine plume was transported and maintained at elevated levels through heterogeneous reactions on colocated supermicron aerosol particles, independent of surface snowpack bromine chemistry. This chemical transport mechanism explains the large spatial extents often observed for reactive bromine chemistry, which impacts atmospheric composition and pollutant fate across the Arctic region, beyond areas of initial snowpack halogen production. The possibility of BrO enhancements disconnected from the surface potentially contributes to sustaining BrO in the free troposphere and must also be considered in the interpretation of satellite BrO column observations, particularly in the context of the rapidly changing Arctic sea ice and snowpack.http://www.atmos-chem-phys.net/17/7567/2017/acp-17-7567-2017.pdf
spellingShingle P. K. Peterson
D. Pöhler
H. Sihler
H. Sihler
J. Zielcke
S. General
U. Frieß
U. Platt
U. Platt
W. R. Simpson
S. V. Nghiem
P. B. Shepson
B. H. Stirm
S. Dhaniyala
T. Wagner
D. R. Caulton
J. D. Fuentes
K. A. Pratt
K. A. Pratt
Observations of bromine monoxide transport in the Arctic sustained on aerosol particles
Atmospheric Chemistry and Physics
title Observations of bromine monoxide transport in the Arctic sustained on aerosol particles
title_full Observations of bromine monoxide transport in the Arctic sustained on aerosol particles
title_fullStr Observations of bromine monoxide transport in the Arctic sustained on aerosol particles
title_full_unstemmed Observations of bromine monoxide transport in the Arctic sustained on aerosol particles
title_short Observations of bromine monoxide transport in the Arctic sustained on aerosol particles
title_sort observations of bromine monoxide transport in the arctic sustained on aerosol particles
url http://www.atmos-chem-phys.net/17/7567/2017/acp-17-7567-2017.pdf
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