Overview of the 2007 and 2008 campaigns conducted as part of the Greenland Summit Halogen-HO x Experiment (GSHOX)

Abstract. From 10 May through 17 June 2007 and 6 June through 9 July 2008 intensive sampling campaigns at Summit, Greenland confirmed that active bromine chemistry is occurring in and above the snow pack at the highest part of the Greenland ice sheet (72°36´ N, 38°25´ W and 3.2 km above sea level). Direct measurements found BrO and soluble gas phase Br − mixing ratios in the low pptv range on many days (maxima −3 of gaseous elemental mercury (GEM) to reactive gaseous mercury (RGM) and enhanced OH relative to HO 2 plus RO 2 confirm that active bromine chemistry is impacting chemical cycles even at such low abundances of reactive bromine species. However, it does not appear that Br y chemistry can fully account for observed perturbations to HO x partitioning, suggesting unknown additional chemical processes may be important in this unique environment, or that our understanding of coupled NO x -HO x -Br y chemistry above sunlit polar snow is incomplete. Rapid transport from the north Atlantic marine boundary layer occasionally caused enhanced BrO at Summit (just two such events observed during the 12 weeks of sampling over the two seasons). In general observed reactive bromine was linked to activation of bromide (Br − ) in, and release of reactive bromine from, the snowpack. A coupled snow-atmosphere model simulated observed NO and BrO at Summit during a three day interval when winds were weak. The source of Br − in surface and near surface snow at Summit is not entirely clear, but concentrations were observed to increase when stronger vertical mixing brought free tropospheric air to the surface. Reactive Br y mixing ratios above the snow often increased in the day or two following increases in snow concentration, but this response was not consistent. On seasonal time scales concentrations of Br − in snow and reactive bromine in the air were directly related.

[1]  F. Hendrick,et al.  Resolution of an important discrepancy between remote and in-situ measurements of tropospheric BrO during Antarctic enhancements , 2012 .

[2]  Jennie L. Thomas,et al.  Modeling chemistry in and above snow at Summit, Greenland – Part 2: Impact of snowpack chemistry on the oxidation capacity of the boundary layer , 2012 .

[3]  Jennie L. Thomas,et al.  Longpath DOAS observations of surface BrO at Summit, Greenland , 2011 .

[4]  J. Curry,et al.  Analysis of satellite-derived Arctic tropospheric BrO columns in conjunction with aircraft measurements during ARCTAS and ARCPAC , 2011 .

[5]  Jennie L. Thomas,et al.  Observations of hydroxyl and peroxy radicals and the impact of BrO at Summit, Greenland in 2007 and 2008 , 2011 .

[6]  G. Huey,et al.  Temperature and sunlight controls of mercury oxidation and deposition atop the Greenland ice sheet , 2011 .

[7]  Jennie L. Thomas,et al.  Modeling chemistry in and above snow at Summit, Greenland – Part 1: Model description and results , 2010 .

[8]  Nicolas Theys,et al.  Global observations of tropospheric BrO columns using GOME-2 satellite data , 2010 .

[9]  Xiong Liu,et al.  A new interpretation of total column BrO during Arctic spring , 2010 .

[10]  L. Ziemba,et al.  Bromide and other ions in the snow, firn air, and atmospheric boundary layer at Summit during GSHOX , 2010 .

[11]  R. Griffin,et al.  Observations of particle growth at a remote, Arctic site , 2010 .

[12]  A. Stohl,et al.  An assessment of the polar HOx photochemical budget based on 2003 Summit Greenland field observations , 2007 .

[13]  P. Shepson,et al.  An overview of snow photochemistry: evidence, mechanisms and impacts , 2007 .

[14]  D. Blake,et al.  An overview of air-snow exchange at Summit, Greenland : Recent experiments and findings , 2007 .

[15]  J. Peischl,et al.  Observations of hydroxyl and the sum of peroxy radicals at Summit, Greenland during summer 2003 , 2007 .

[16]  J. Dibb Vertical mixing above Summit, Greenland: Insights into seasonal and high frequency variability from the radionuclide tracers 7Be and 210Pb , 2007 .

[17]  J. Dibb,et al.  Seasonal distributions of fine aerosol sulfate in the North American Arctic basin during TOPSE : Tropospheric Ozone Production about the Spring Equinox (TOPSE) , 2003 .

[18]  K. Steffen,et al.  Vertical fluxes of NOx, HONO, and HNO3 above the snowpack at Summit, Greenland , 2002 .

[19]  P. Shepson,et al.  Impacts of snowpack emissions on deduced levels of OH and peroxy radicals at Summit, Greenland , 2002 .

[20]  Barry Lefer,et al.  Unexpected high levels of NO observed at South Pole , 2001 .

[21]  P. Shepson,et al.  Is the Arctic Surface Layer a Source and Sink of NOx in Winter/Spring? , 2000 .

[22]  A. Jones,et al.  Speciation and rate of photochemical NO and NO2 production in Antarctic snow , 2000 .

[23]  C. T. McElroy,et al.  Evidence for bromine monoxide in the free troposphere during the Arctic polar sunrise , 1999, Nature.

[24]  R. Honrath,et al.  Evidence of NOx production within or upon ice particles in the Greenland snowpack , 2023 .