Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Modelling the coupled mercury-halogen-ozone cycle in the central Arctic during spring

Journal Article · · Elementa
 [1];  [1];  [2];  [1];  [3];  [4];  [5];  [6];  [7];  [4];  [8];  [9];  [10];  [11];  [12];  [4];  [1];  [13];  [1];  [8] more »;  [8];  [7];  [11];  [14];  [15];  [16];  [3];  [10];  [6];  [5];  [9];  [17];  [17];  [18];  [19];  [7] « less
  1. Univ. of Grenoble Alpes, Grenoble (France)
  2. Univ. of Grenoble Alpes, Grenoble (France); Ecole Polytechnique Federale Lausanne (EPFL) (Switzerland); Univ. of Colorado, Boulder, CO (United States)
  3. Bigelow Laboratory for Ocean Sciences, East Boothbay, ME (United States)
  4. Univ. of Colorado, Boulder, CO (United States); National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Physical Sciences Laboratory
  5. Ecole Polytechnique Federale Lausanne (EPFL) (Switzerland)
  6. Institute of Physical Chemistry Rocasolano, Madrid (Spain)
  7. Univ. of Bremen (Germany)
  8. Univ. of Helsinki (Finland)
  9. Aarhus Univ., Roskilde (Denmark)
  10. Alfred Wegener Inst. for Polar and Marine Research, Potsdam (Germany)
  11. Environment and Climate Change Canada, Dorval, QC (Canada)
  12. Univ. of Colorado, Boulder, CO (United States); Boulder AIR, CO (United States)
  13. Univ. of Helsinki (Finland); Cyprus Institute, Nicosia (Cyprus)
  14. Indian Institute of Tropical Meteorology, Pune (India)
  15. Sorbonne Univ., Paris (France)
  16. Norwegian Inst. for Air Research (NILU), Kjeller (Norway)
  17. Environment and Climate Change Canada, Toronto, ON (Canada)
  18. Univ. of California, Los Angeles, CA (United States)
  19. Meteorology Synthesizing Centre-East, Moscow (Russian Federation)
+ Show Author Affiliations

Near-surface mercury and ozone depletion events occur in the lowest part of the atmosphere during Arctic spring. Mercury depletion is the first step in a process that transforms long-lived elemental mercury to more reactive forms within the Arctic that are deposited to the cryosphere, ocean, and other surfaces, which can ultimately get integrated into the Arctic food web. Depletion of both mercury and ozone occur due to the presence of reactive halogen radicals that are released from snow, ice, and aerosols. In this work, we added a detailed description of the Arctic atmospheric mercury cycle to our recently published version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem 4.3.3) that includes Arctic bromine and chlorine chemistry and activation/recycling on snow and aerosols. The major advantage of our modelling approach is the online calculation of bromine concentrations and emission/recycling that is required to simulate the hourly and daily variability of Arctic mercury depletion. We used this model to study coupling between reactive cycling of mercury, ozone, and bromine during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) spring season in 2020 and evaluated results compared to land-based, ship-based, and remote sensing observations. The model predicts that elemental mercury oxidation is driven largely by bromine chemistry and that particulate mercury is the major form of oxidized mercury. The model predicts that the majority (74%) of oxidized mercury deposited to land-based snow is re-emitted to the atmosphere as gaseous elemental mercury, while a minor fraction (4%) of oxidized mercury that is deposited to sea ice is re-emitted during spring. Our work demonstrates that hourly differences in bromine/ozone chemistry in the atmosphere must be considered to capture the springtime Arctic mercury cycle, including its integration into the cryosphere and ocean.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Contributing Organization:
Pacific Northwest National Laboratory (PNNL); Brookhaven National Laboratory (BNL); Argonne National Laboratory (ANL)
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1984453
Journal Information:
Elementa, Vol. 11, Issue 1; ISSN 2325-1026
Publisher:
University of California PressCopyright Statement
Country of Publication:
United States
Language:
English

References (154)

Halogen activation via interactions with environmental ice and snow in the polar lower troposphere and other regions journal January 2012
Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition journal January 2012
Year-round trace gas measurements in the central Arctic during the MOSAiC expedition journal November 2022
Chemical cycling and deposition of atmospheric mercury in polar regions: review of recent measurements and comparison with models journal August 2016
Mercury isotope evidence for Arctic summertime re-emission of mercury from the cryosphere journal August 2022
Mercury Physicochemical and Biogeochemical Transformation in the Atmosphere and at Atmospheric Interfaces: A Review and Future Directions journal February 2015
Accurate Global Potential Energy Surface and Reaction Dynamics for the Ground State of HgBr 2 journal October 2005
Arctic air pollution: An overview of current knowledge journal January 1986
Ozone destruction and photochemical reactions at polar sunrise in the lower Arctic atmosphere journal July 1988
Substantial contribution of iodine to Arctic ozone destruction journal September 2022
A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli journal January 2015
Ten-year trends in atmospheric mercury concentrations, meteorological effects and climate variables at Zeppelin, Ny-Ålesund journal July 2013
Depletion of lower tropospheric ozone during Arctic spring: The Polar Sunrise Experiment 1988 journal January 1990
The mass balance of mercury in the springtime arctic environment journal January 2006
The Solubility of Mercury and Some Sparingly Soluble Mercury Salts in Water and Aqueous Electrolyte Solutions
  • Clever, H. Lawrence; Johnson, Susan A.; Derrick, M. Elizabeth
  • Journal of Physical and Chemical Reference Data, Vol. 14, Issue 3 https://doi.org/10.1063/1.555732
journal July 1985
GEM fluxes and atmospheric mercury concentrations (GEM, RGM and Hgp) in the Canadian Arctic at Alert, Nunavut, Canada (February–June 2005) journal October 2007
A central arctic extreme aerosol event triggered by a warm air-mass intrusion journal September 2022
Arctic mercury cycling journal March 2022
Arctic atmospheric mercury: Sources and changes journal September 2022
Modeling the OH-Initiated Oxidation of Mercury in the Global Atmosphere without Violating Physical Laws journal December 2019
Thermodynamics of reactions of ClHg and BrHg radicals with atmospherically abundant free radicals journal January 2012
Laboratory simulation of Hg0 emissions from a snowpack journal February 2007
Diurnal Cycles of Gaseous Mercury within the Snowpack at Kuujjuarapik/Whapmagoostui, Québec, Canada journal June 2003
Deposition of Mercury Species in the Ny-Ålesund Area (79°N) and Their Transfer during Snowmelt journal December 2009
Mercury Isotopes Reveal Atmospheric Gaseous Mercury Deposition Directly to the Arctic Coastal Snowpack journal March 2019
The fate of mercury in Arctic terrestrial and aquatic ecosystems, a review journal January 2012
Mercury as a Global Pollutant: Sources, Pathways, and Effects journal May 2013
The behavior of mercury in the cryosphere: A review of what we know from observations journal March 2011
Long range transport of mercury to the Arctic and across Canada journal July 2010
How relevant is the deposition of mercury onto snowpacks? – Part 2: A modeling study journal October 2012
The Chemistry Mechanism in the Community Earth System Model Version 2 (CESM2) journal April 2020
Polar boundary layer bromine explosion and ozone depletion events in the chemistry–climate model EMAC v2.52: implementation and evaluation of AirSnow algorithm journal March 2018
Snow-to-air exchanges of mercury in an Arctic seasonal snow pack in Ny-Ålesund, Svalbard journal December 2005
Atmospheric mercury depletion event study in Ny-Alesund (Svalbard) in spring 2005. Deposition and transformation of Hg in surface snow during springtime journal July 2008
Factors driving mercury variability in the Arctic atmosphere and ocean over the past 30 years journal December 2013
Riverine source of Arctic Ocean mercury inferred from atmospheric observations journal May 2012
Photodissociation Mechanisms of Major Mercury(II) Species in the Atmospheric Chemical Cycle of Mercury journal January 2020
Development and application of a regional-scale atmospheric mercury model based on WRF/Chem: a Mediterranean area investigation journal October 2013
The reaction between HgBr and O3: kinetic study and atmospheric implications journal January 2022
A Theoretical Study of the Oxidation of Hg 0 to HgBr 2 in the Troposphere journal March 2004
Correction to A Theoretical Study of the Oxidation of Hg0 to HgBr2 in the Troposphere journal April 2012
Evaluation of Six Atmospheric Reanalyses over Arctic Sea Ice from Winter to Early Summer journal June 2019
The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions journal January 2012
Measuring and modeling mercury in the atmosphere: a critical review journal May 2015
Do We Understand What the Mercury Speciation Instruments Are Actually Measuring? Results of RAMIX journal January 2013
Temporal and spatial characteristics of ozone depletion events from measurements in the Arctic journal January 2014
Ozone depletion events in the Arctic spring of 2019: a new modeling approach to bromine emissions journal October 2022
Time-dependent 3D simulations of tropospheric ozone depletion events in the Arctic spring using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) journal May 2021
Methylated Mercury Species in Canadian High Arctic Marine Surface Waters and Snowpacks journal August 2007
Global atmospheric model for mercury including oxidation by bromine atoms journal January 2010
Observations of BrO and its vertical distribution during surface ozone depletion at Alert journal May 2002
A new mechanism for atmospheric mercury redox chemistry: implications for the global mercury budget journal January 2017
Wintertime enhancements of sea salt aerosol in polar regions consistent with a sea ice source from blowing snow journal January 2017
Evaluating the impact of blowing-snow sea salt aerosol on springtime BrO and O3 in the Arctic journal June 2020
Using CALIOP to constrain blowing snow emissions of sea salt aerosols over Arctic and Antarctic sea ice journal November 2018
Comparison of Gaseous Oxidized Hg Measured by KCl-Coated Denuders, and Nylon and Cation Exchange Membranes journal May 2013
Our current understanding of major chemical and physical processes affecting mercury dynamics in the atmosphere and at the air-water/terrestrial interfaces book January 2009
Radiative forcing by long-lived greenhouse gases: Calculations with the AER radiative transfer models journal January 2008
Heterogeneous chemistry and tropospheric ozone journal January 2000
The NCEP/NCAR 40-Year Reanalysis Project journal March 1996
Fluxes of gaseous elemental mercury (GEM) in the High Arctic during atmospheric mercury depletion events (AMDEs) journal May 2018
BrHgO• + CO: Analogue of OH + CO and Reduction Path for Hg(II) in the Atmosphere journal September 2020
Rapid Reduction and Reemission of Mercury Deposited into Snowpacks during Atmospheric Mercury Depletion Events at Churchill, Manitoba, Canada journal November 2006
Global anthropogenic emissions of particulate matter including black carbon journal January 2017
Development of an autonomous sea ice tethered buoy for the study of ocean-atmosphere-sea ice-snow pack interactions: the O-buoy journal February 2010
Polar Research and Supply Vessel POLARSTERN operated by the Alfred-Wegener-Institute journal January 2017
The chemical composition of surface snow in the Arctic: Examining marine, terrestrial, and atmospheric influences journal April 2012
Photo‐induced Hg(II) reduction in snow from the remote and temperate Experimental Lakes Area (Ontario, Canada) journal March 2003
The Role of Mercury Redox Reactions in Snow on Snow-to-Air Mercury Transfer journal December 2001
Importance of Ultraviolet Radiation in the Photodemethylation of Methylmercury in Freshwater Ecosystems journal August 2009
Dynamic Oxidation of Gaseous Mercury in the Arctic Troposphere at Polar Sunrise journal March 2002
Formation of Reactive Gaseous Mercury in the Arctic: Evidence of Oxidation of Hg?? to Gas-Phase Hg-II Compounds after Arctic Sunrise book January 2001
Atmospheric Mercury Speciation:  Concentrations and Behavior of Reactive Gaseous Mercury in Ambient Air journal January 1998
Atmospheric mercury-a review journal July 1985
Ground-based imaging differential optical absorption spectroscopy of atmospheric gases journal January 2004
Magnification of atmospheric mercury deposition to polar regions in springtime: The link to tropospheric ozone depletion chemistry journal September 2001
Updated trends for atmospheric mercury in the Arctic: 1995–2018 journal September 2022
Dynamics of snow-air mercury exchange at Ny Ålesund during springtime 2011 journal January 2013
Mercury in Arctic snow: Quantifying the kinetics of photochemical oxidation and reduction journal March 2015
Photoreducible Mercury Loss from Arctic Snow Is Influenced by Temperature and Snow Age journal October 2015
Increasing chloride concentration causes retention of mercury in melted Arctic snow due to changes in photoreduction kinetics journal June 2018
Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic journal January 2017
Implementation and Impacts of Surface and Blowing Snow Sources of Arctic Bromine Activation Within WRF‐Chem 4.1.1 journal July 2021
Impact of Cloud Microphysics on the Development of Trailing Stratiform Precipitation in a Simulated Squall Line: Comparison of One- and Two-Moment Schemes journal March 2009
Development of an Improved Turbulence Closure Model for the Atmospheric Boundary Layer journal January 2009
Overview of the MOSAiC expedition journal January 2022
Surface ozone measurements in clean air journal January 1981
Fate of Springtime Atmospheric Reactive Mercury: Concentrations and Deposition at Zeppelin, Svalbard journal October 2021
Mercury and trace metal wet deposition across five stations in Alaska: controlling factors, spatial patterns, and source regions journal May 2019
Overview: Integrative and Comprehensive Understanding on Polar Environments (iCUPE) – concept and initial results journal January 2020
Snowpack measurements suggest role for multi-year sea ice regions in Arctic atmospheric bromine and chlorine chemistry journal January 2019
Observations of bromine monoxide transport in the Arctic sustained on aerosol particles journal June 2017
Atmospheric composition in the European Arctic and 30 years of the Zeppelin Observatory, Ny-Ålesund journal March 2022
The role of halogen species in the troposphere journal July 2003
Differential Absorption Spectroscopy book January 2008
Atmospheric mercury speciation and deposition in the Bay St. François wetlands journal January 2004
Mercury distribution, partitioning and speciation in coastal vs. inland High Arctic snow journal July 2007
Redox transformations of mercury in an Arctic snowpack at springtime journal December 2004
Iodine oxide in the global marine boundary layer journal January 2015
Wet deposition of mercury in the U.S. and Canada, 1996–2005: Results and analysis of the NADP mercury deposition network (MDN) journal September 2009
Overview of the MOSAiC expedition: Physical oceanography journal January 2022
How Well Are We Measuring Snow: The NOAA/FAA/NCAR Winter Precipitation Test Bed journal June 2012
Sea ice as a source of sea salt aerosol to Greenland ice cores: a model-based study journal January 2017
Gas-Phase Photolysis of Hg(I) Radical Species: A New Atmospheric Mercury Reduction Process journal May 2019
Photoreduction of gaseous oxidized mercury changes global atmospheric mercury speciation, transport and deposition journal November 2018
Technical note: Simulating chemical systems in Fortran90 and Matlab with the Kinetic PreProcessor KPP-2.1 journal January 2006
Wet deposition mercury fluxes in the Canadian sub-Arctic and southern Alberta, measured using an automated precipitation collector adapted to cold regions journal April 2010
Arctic springtime depletion of mercury journal July 1998
Summary report: first international Arctic atmospheric mercury research workshop journal June 2003
Mass-Transport Considerations Pertinent to Aqueous Phase Reactions of Gases in Liquid-Water Clouds book January 1986
Global Source Attribution for Mercury Deposition in the United States journal December 2003
Global Biogeochemical Cycling of Mercury: A Review journal November 2009
Global 3-D land-ocean-atmosphere model for mercury: Present-day versus preindustrial cycles and anthropogenic enrichment factors for deposition: GLOBAL 3-D LAND-OCEAN-ATMOSPHERE MODEL FOR MERCURY journal May 2008
First high-resolution BrO column retrievals from TROPOMI journal May 2019
Improved Mechanistic Model of the Atmospheric Redox Chemistry of Mercury journal August 2021
Overview of the MOSAiC expedition: Atmosphere journal January 2022
Tropospheric Halogen Chemistry: Sources, Cycling, and Impacts journal February 2015
Horizontal and vertical structure of reactive bromine events probed by bromine monoxide MAX-DOAS journal August 2017
Halogens and their role in polar boundary-layer ozone depletion journal January 2007
Fluxes of reactive gaseous mercury measured with a newly developed method using relaxed eddy accumulation journal September 2006
Fate of Elemental Mercury in the Arctic during Atmospheric Mercury Depletion Episodes and the Load of Atmospheric Mercury to the Arctic journal March 2004
Variability in gaseous elemental mercury at Villum Research Station, Station Nord, in North Greenland from 1999 to 2017 journal January 2020
Comparison of mercury concentrations measured at several sites in the Southern Hemisphere journal March 2015
Circumpolar transport and air-surface exchange of atmospheric mercury at Ny-Ålesund (79° N), Svalbard, spring 2002 journal January 2007
Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling journal June 2015
Five-year records of mercury wet deposition flux at GMOS sites in the Northern and Southern hemispheres journal February 2017
Dynamic exchange of gaseous elemental mercury during polar night and day journal November 2009
Development and application of an updated geospatial distribution model for gridding 2015 global mercury emissions journal August 2019
Atmospheric mercury over sea ice during the OASIS-2009 campaign journal July 2013
Atmospheric mercury speciation and mercury in snow over time at Alert, Canada journal March 2014
Atmospheric mercury concentrations: measurements and profiles near snow and ice surfaces in the Canadian Arctic during Alert 2000 journal May 2002
The relative importance of chlorine and bromine radicals in the oxidation of atmospheric mercury at Barrow, Alaska journal March 2012
A review of uncertainties in atmospheric modeling of mercury chemistry I. Uncertainties in existing kinetic parameters – Fundamental limitations and the importance of heterogeneous chemistry journal October 2011
A review of the sources of uncertainties in atmospheric mercury modeling II. Mercury surface and heterogeneous chemistry – A missing link journal January 2012
Comparison of model and ground observations finds snowpack and blowing snow aerosols both contribute to Arctic tropospheric reactive bromine journal November 2022
Global observations of tropospheric BrO columns using GOME-2 satellite data journal January 2011
Analysis of reactive bromine production and ozone depletion in the Arctic boundary layer using 3-D simulations with GEM-AQ: inference from synoptic-scale patterns journal April 2011
Air–snowpack exchange of bromine, ozone and mercury in the springtime Arctic simulated by the 1-D model PHANTAS – Part 1: In-snow bromine activation and its impact on ozone journal January 2014
Multi-model study of mercury dispersion in the atmosphere: atmospheric processes and model evaluation journal January 2017
Snowfall and snow accumulation during the MOSAiC winter and spring seasons journal June 2022
Spatial and temporal distribution of enhanced boundary layer BrO concentrations measured by the GOME instrument aboard ERS-2 journal October 2001
Direct detection of atmospheric atomic bromine leading to mercury and ozone depletion journal June 2019
Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models journal January 1989
The Fire INventory from NCAR (FINN): a high resolution global model to estimate the emissions from open burning journal January 2011
Fast-J: Accurate Simulation of In- and Below-Cloud Photolysis in Tropospheric Chemical Models journal January 2000
Gas-particle partitioning of atmospheric reactive mercury and its contribution to particle bound mercury in a coastal city of the Yangtze River Delta, China journal October 2020
Pan-Arctic surface ozone: modelling vs. measurements journal December 2020
Sea salt aerosol production via sublimating wind-blown saline snow particles over sea ice: parameterizations and relevant microphysical mechanisms journal July 2019
Sea salt aerosol production and bromine release: Role of snow on sea ice journal January 2008
Snow-sourced bromine and its implications for polar tropospheric ozone journal August 2010
Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) journal January 2008
Estimation of speciated and total mercury dry deposition at monitoring locations in eastern and central North America journal May 2012
A review of current knowledge concerning dry deposition of atmospheric mercury journal December 2009
Earth system modeling of mercury using CESM2 – Part 1: Atmospheric model CAM6-Chem/Hg v1.0 journal May 2022

Similar Records

Related Subjects

54 ENVIRONMENTAL SCIENCES
Arctic
Ozone
Mercury
Bromine
Cryosphere
Atmosphere