Preprints
https://doi.org/10.5194/acp-2021-782
https://doi.org/10.5194/acp-2021-782

  27 Sep 2021

27 Sep 2021

Review status: this preprint is currently under review for the journal ACP.

Exploring DMS oxidation and implications for global aerosol radiative forcing

Ka Ming Fung1, Colette L. Heald1,2, Jesse H. Kroll1, Siyuan Wang3, Duseong S. Jo4, Andrew Gettelman4, Zheng Lu5, Xiaohong Liu5, Rahul A. Zaveri6, Eric Apel4, Donald R. Blake7, Jose-Luis Jimenez8, Pedro Campuzano-Jost8, Patrick Veres3, Timothy S. Bates9, John E. Shilling10, and Maria Zawadowicz11 Ka Ming Fung et al.
  • 1Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
  • 2Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA, USA
  • 3Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
  • 4Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
  • 5Department of Atmospheric Sciences, Texas A&M University, College Station, TX, USA
  • 6Pacific Northwest National Laboratory, Richland, WA, USA
  • 7Department of Chemistry, University of California, Irvine, CA, USA
  • 8Department of Chemistry & Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 9The Cooperative Institute for Climate, Ocean, and Ecosystem Studies, College of the Environment, University of Washington, Seattle, WA, USA
  • 10Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USA
  • 11Environmental and Climate Sciences Department, Brookhaven National Laboratory, Upton, NY, USA

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway as well as the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden, as well as the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg-S (+29 %) and 582 Gg-S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11  W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2 with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading, as well as the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

Ka Ming Fung et al.

Status: open (until 08 Nov 2021)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse

Ka Ming Fung et al.

Ka Ming Fung et al.

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Short summary
Understanding the natural aerosol burden in the pre-industrial is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of DMS oxidation (implemented in an atmospheric model named CAM6-chem) could help us better estimate the present-day and pre-industrial concentrations of sulfate and other relevant chemicals as well as the resulting aerosol radiative impacts.
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