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The role of snow in controlling halogen chemistry and boundary layer oxidation during Arctic spring: A 1D modelling case study
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  • Shaddy Ahmed,
  • Jennie L Thomas,
  • Kathleen Tuite,
  • Jochen Stutz,
  • Frank Flocke,
  • John Orlando,
  • Rebecca S. Hornbrook,
  • Eric C Apel,
  • Louisa K. Emmons,
  • Detlev Helmig,
  • Patrick Boylan,
  • L. Gregory Huey,
  • Samuel R Hall,
  • Kirk Ullmann,
  • Christopher A. Cantrell,
  • Alan Fried
Shaddy Ahmed
Université de Grenoble Alpes, CNRS, IRD, Grenoble INP, IGE

Corresponding Author:[email protected]

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Jennie L Thomas
L'Institut des Géosciences de l'Environnement (IGE)
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Kathleen Tuite
University of California Los Angeles
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Jochen Stutz
University of California Los Angeles
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Frank Flocke
National Center for Atmospheric Research (UCAR)
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John Orlando
National Center for Atmospheric Research (UCAR)
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Rebecca S. Hornbrook
National Center for Atmospheric Research (UCAR)
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Eric C Apel
NCAR
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Louisa K. Emmons
National Center for Atmospheric Research (UCAR)
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Detlev Helmig
Boulder Air LLC
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Patrick Boylan
National Center for Atmospheric Research (UCAR)
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L. Gregory Huey
Georgia Inst of Techn.
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Samuel R Hall
National Center for Atmospheric Research (UCAR)
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Kirk Ullmann
National Center for Atmospheric Research (UCAR)
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Christopher A. Cantrell
University of Colorado Boulder
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Alan Fried
University of Colorado Boulder
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Abstract

Reactive chlorine and bromine species emitted from snow and aerosols can significantly alter the oxidative capacity of the polar boundary layer. However, halogen production mechanisms from snow remain highly uncertain, making it difficult for most models to include descriptions of halogen snow emissions and to understand the impact on atmospheric chemistry. We investigate the influence of Arctic halogen emissions from snow on boundary layer oxidation processes using a one-dimensional atmospheric chemistry and transport model (PACT-1D). To understand the combined impact of snow emissions and boundary layer dynamics on atmospheric chemistry, we model \ch{Cl2} and \ch{Br2} primary emissions from snow and include heterogeneous recycling of halogens on both snow and aerosols. We focus on a two-day case study from the 2009 Ocean-Atmosphere-Sea Ice-Snowpack (OASIS) campaign at Utqia\.gvik, Alaska. The model reproduces both the diurnal cycle and high quantity of \ch{Cl2} observed, along with the measured concentrations of \ch{Br2}, \ch{BrO}, and \ch{HOBr}. Due to the combined effects of emissions, recycling, vertical mixing, and atmospheric chemistry, reactive chlorine is confined to the lowest 15 m of the atmosphere, while bromine impacts chemistry up to the boundary layer height. Upon including halogen emissions and recycling, the concentration of \ch{HO_x} (\ch{HO_x} = \ch{OH}+\ch{HO2}) at the surface increases by as much as a factor of 30 at mid-day. The change in \ch{HO_x} due to halogen chemistry, as well as chlorine atoms derived from snow emissions, significantly reduce volatile organic compound (VOC) lifetimes within a shallow layer near the surface.
16 Mar 2022Published in Journal of Geophysical Research: Atmospheres volume 127 issue 5. 10.1029/2021JD036140