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Title: The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings

Abstract

Atmospheric marine aerosol particles impact Earth's albedo and climate. These particles can be primary or secondary and come from a variety of sources, including sea salt, dissolved organic matter, volatile organic compounds, and sulfur-containing compounds. Dimethylsulfide (DMS) marine emissions contribute greatly to the global biogenic sulfur budget, and its oxidation products can contribute to aerosol mass, specifically as sulfuric acid and methanesulfonic acid (MSA). Further, sulfuric acid is a known nucleating compound, and MSA may be able to participate in nucleation when bases are available. As DMS emissions, and thus MSA and sulfuric acid from DMS oxidation, may have changed since pre-industrial times and may change in a warming climate, it is important to characterize and constrain the climate impacts of both species. Currently, global models that simulate aerosol size distributions include contributions of sulfate and sulfuric acid from DMS oxidation, but to our knowledge, global models typically neglect the impact of MSA on size distributions. In this study, we use the GEOS-Chem-TOMAS (GC-TOMAS) global aerosol microphysics model to determine the impact on aerosol size distributions and subsequent aerosol radiative effects from including MSA in the size-resolved portion of the model. The effective equilibrium vapor pressure of MSA is currentlymore » uncertain, and we use the Extended Aerosol Inorganics Model (E-AIM) to build a parameterization for GC-TOMAS of MSA's effective volatility as a function of temperature, relative humidity, and available gas-phase bases, allowing MSA to condense as an ideally nonvolatile or semivolatile species or too volatile to condense. We also present two limiting cases for MSA's volatility, assuming that MSA is always ideally nonvolatile (irreversible condensation) or that MSA is always ideally semivolatile (quasi-equilibrium condensation but still irreversible condensation). We further present simulations in which MSA participates in binary and ternary nucleation with the same efficacy as sulfuric acid whenever MSA is treated as ideally nonvolatile. When using the volatility parameterization described above (both with and without nucleation), including MSA in the model changes the global annual averages at 900 hPa of submicron aerosol mass by 1.2 %, N3 (number concentration of particles greater than 3 nm in diameter) by -3.9 % (non-nucleating) or 112.5 % (nucleating), N80 by 0.8 % (non-nucleating) or 2.1 % (nucleating), the cloud-albedo aerosol indirect effect (AIE) by -8.6 mW m-2 (non-nucleating) or -26 mW m-2 (nucleating), and the direct radiative effect (DRE) by -15 mW m-2 (non-nucleating) or -14 mW m-2 (nucleating). The sulfate and sulfuric acid from DMS oxidation produces 4–6 times more submicron mass than MSA does, leading to an ~10 times stronger cooling effect in the DRE. But the changes in N80 are comparable between the contributions from MSA and from DMS-derived sulfate/sulfuric acid, leading to comparable changes in the cloud-albedo AIE. Model–measurement comparisons with the Heintzenberg et al. (2000) dataset over the Southern Ocean indicate that the default model has a missing source or sources of ultrafine particles: the cases in which MSA participates in nucleation (thus increasing ultrafine number) most closely match the Heintzenberg distributions, but we cannot conclude nucleation from MSA is the correct reason for improvement. Model–measurement comparisons with particle-phase MSA observed with a customized Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS) from the ATom campaign show that cases with the MSA volatility parameterizations (both with and without nucleation) tend to fit the measurements the best (as this is the first use of MSA measurements from ATom, we provide a detailed description of these measurements and their calibration). However, no one model sensitivity case shows the best model–measurement agreement for both Heintzenberg and the ATom campaigns. As there are uncertainties in both MSA's behavior (nucleation and condensation) and the DMS emissions inventory, further studies on both fronts are needed to better constrain MSA's past, current, and future impacts upon the global aerosol size distribution and radiative forcing.« less

Authors:
ORCiD logo; ORCiD logo; ; ORCiD logo; ORCiD logo; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Colorado State Univ., Fort Collins, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Aeronautics and Space Administration (NASA); National Oceanic and Atmospheric Administration (NOAA); Natural Sciences and Engineering Research Council of Canada (NSERC)
OSTI Identifier:
1499057
Alternate Identifier(s):
OSTI ID: 1611664
Grant/Contract Number:  
SC0011780
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 19 Journal Issue: 5; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences

Citation Formats

Hodshire, Anna L., Campuzano-Jost, Pedro, Kodros, John K., Croft, Betty, Nault, Benjamin A., Schroder, Jason C., Jimenez, Jose L., and Pierce, Jeffrey R. The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings. Germany: N. p., 2019. Web. doi:10.5194/acp-19-3137-2019.
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Hodshire, Anna L., Campuzano-Jost, Pedro, Kodros, John K., Croft, Betty, Nault, Benjamin A., Schroder, Jason C., Jimenez, Jose L., & Pierce, Jeffrey R. The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings. Germany. https://doi.org/10.5194/acp-19-3137-2019
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Hodshire, Anna L., Campuzano-Jost, Pedro, Kodros, John K., Croft, Betty, Nault, Benjamin A., Schroder, Jason C., Jimenez, Jose L., and Pierce, Jeffrey R. Tue . "The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings". Germany. https://doi.org/10.5194/acp-19-3137-2019.
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@article{osti_1499057,
title = {The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings},
author = {Hodshire, Anna L. and Campuzano-Jost, Pedro and Kodros, John K. and Croft, Betty and Nault, Benjamin A. and Schroder, Jason C. and Jimenez, Jose L. and Pierce, Jeffrey R.},
abstractNote = {Atmospheric marine aerosol particles impact Earth's albedo and climate. These particles can be primary or secondary and come from a variety of sources, including sea salt, dissolved organic matter, volatile organic compounds, and sulfur-containing compounds. Dimethylsulfide (DMS) marine emissions contribute greatly to the global biogenic sulfur budget, and its oxidation products can contribute to aerosol mass, specifically as sulfuric acid and methanesulfonic acid (MSA). Further, sulfuric acid is a known nucleating compound, and MSA may be able to participate in nucleation when bases are available. As DMS emissions, and thus MSA and sulfuric acid from DMS oxidation, may have changed since pre-industrial times and may change in a warming climate, it is important to characterize and constrain the climate impacts of both species. Currently, global models that simulate aerosol size distributions include contributions of sulfate and sulfuric acid from DMS oxidation, but to our knowledge, global models typically neglect the impact of MSA on size distributions. In this study, we use the GEOS-Chem-TOMAS (GC-TOMAS) global aerosol microphysics model to determine the impact on aerosol size distributions and subsequent aerosol radiative effects from including MSA in the size-resolved portion of the model. The effective equilibrium vapor pressure of MSA is currently uncertain, and we use the Extended Aerosol Inorganics Model (E-AIM) to build a parameterization for GC-TOMAS of MSA's effective volatility as a function of temperature, relative humidity, and available gas-phase bases, allowing MSA to condense as an ideally nonvolatile or semivolatile species or too volatile to condense. We also present two limiting cases for MSA's volatility, assuming that MSA is always ideally nonvolatile (irreversible condensation) or that MSA is always ideally semivolatile (quasi-equilibrium condensation but still irreversible condensation). We further present simulations in which MSA participates in binary and ternary nucleation with the same efficacy as sulfuric acid whenever MSA is treated as ideally nonvolatile. When using the volatility parameterization described above (both with and without nucleation), including MSA in the model changes the global annual averages at 900 hPa of submicron aerosol mass by 1.2 %, N3 (number concentration of particles greater than 3 nm in diameter) by -3.9 % (non-nucleating) or 112.5 % (nucleating), N80 by 0.8 % (non-nucleating) or 2.1 % (nucleating), the cloud-albedo aerosol indirect effect (AIE) by -8.6 mW m-2 (non-nucleating) or -26 mW m-2 (nucleating), and the direct radiative effect (DRE) by -15 mW m-2 (non-nucleating) or -14 mW m-2 (nucleating). The sulfate and sulfuric acid from DMS oxidation produces 4–6 times more submicron mass than MSA does, leading to an ~10 times stronger cooling effect in the DRE. But the changes in N80 are comparable between the contributions from MSA and from DMS-derived sulfate/sulfuric acid, leading to comparable changes in the cloud-albedo AIE. Model–measurement comparisons with the Heintzenberg et al. (2000) dataset over the Southern Ocean indicate that the default model has a missing source or sources of ultrafine particles: the cases in which MSA participates in nucleation (thus increasing ultrafine number) most closely match the Heintzenberg distributions, but we cannot conclude nucleation from MSA is the correct reason for improvement. Model–measurement comparisons with particle-phase MSA observed with a customized Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS) from the ATom campaign show that cases with the MSA volatility parameterizations (both with and without nucleation) tend to fit the measurements the best (as this is the first use of MSA measurements from ATom, we provide a detailed description of these measurements and their calibration). However, no one model sensitivity case shows the best model–measurement agreement for both Heintzenberg and the ATom campaigns. As there are uncertainties in both MSA's behavior (nucleation and condensation) and the DMS emissions inventory, further studies on both fronts are needed to better constrain MSA's past, current, and future impacts upon the global aerosol size distribution and radiative forcing.},
doi = {10.5194/acp-19-3137-2019},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 5,
volume = 19,
place = {Germany},
year = {Tue Mar 12 00:00:00 EDT 2019},
month = {Tue Mar 12 00:00:00 EDT 2019}
}
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Mineral Dust Entrainment and Deposition (DEAD) model: Description and 1990s dust climatology
journal, January 2003

Model for acid-base chemistry in nanoparticle growth (MABNAG)
journal, January 2013

  • Yli-Juuti, T.; Barsanti, K.; Hildebrandt Ruiz, L.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 24
  • DOI: 10.5194/acp-13-12507-2013

Flux of dimethylsulfide from the oceans: A comparison of updated data sets and flux models
journal, November 2000

  • Kettle, A. J.; Andreae, M. O.
  • Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D22
  • DOI: 10.1029/2000JD900252

Natural aerosol direct and indirect radiative effects: NATURAL AEROSOL RADIATIVE EFFECTS
journal, June 2013

  • Rap, Alexandru; Scott, Catherine E.; Spracklen, Dominick V.
  • Geophysical Research Letters, Vol. 40, Issue 12
  • DOI: 10.1002/grl.50441

Size distribution and chemical composition of marine aerosols: a compilation and review
journal, September 2000

Inversion of aerosol data from the epiphaniometer
journal, January 1991

  • Pandis, Spyros N.; Baltensperger, Urs; Wolfenbarger, J. Kenneth
  • Journal of Aerosol Science, Vol. 22, Issue 4
  • DOI: 10.1016/0021-8502(91)90002-Y

FT-IR product study on the photo-oxidation of dimethyl sulphide in the presence of NOx—temperature dependence
journal, August 2001

Dependence of DMS global sea-air flux distribution on transfer velocity and concentration field type: DMS GLOBAL SEA-AIR FLUX DISTRIBUTION
journal, April 2009

  • Elliott, Scott
  • Journal of Geophysical Research: Biogeosciences, Vol. 114, Issue G2
  • DOI: 10.1029/2008JG000710

Efficiency of cloud condensation nuclei formation from ultrafine particles
journal, January 2007

Representation of nucleation mode microphysics in a global aerosol model with sectional microphysics
journal, January 2013

  • Lee, Y. H.; Pierce, J. R.; Adams, P. J.
  • Geoscientific Model Development, Vol. 6, Issue 4
  • DOI: 10.5194/gmd-6-1221-2013

Abiotic and biotic sources influencing spring new particle formation in North East Greenland
journal, October 2018

Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates
journal, January 2009

Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data
journal, January 2009

  • Ulbrich, I. M.; Canagaratna, M. R.; Zhang, Q.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 9
  • DOI: 10.5194/acp-9-2891-2009

Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer
journal, January 2007

  • Canagaratna, M. R.; Jayne, J. T.; Jimenez, J. L.
  • Mass Spectrometry Reviews, Vol. 26, Issue 2
  • DOI: 10.1002/mas.20115

Influence of oceanic dimethyl sulfide emissions on cloud condensation nuclei concentrations and seasonality over the remote Southern Hemisphere oceans: A global model study
journal, January 2008

  • Korhonen, Hannele; Carslaw, Kenneth S.; Spracklen, Dominick V.
  • Journal of Geophysical Research, Vol. 113, Issue D15
  • DOI: 10.1029/2007JD009718

Vertically resolved concentration and liquid water content of atmospheric nanoparticles at the US DOE Southern Great Plains site
journal, January 2018

  • Chen, Haihan; Hodshire, Anna L.; Ortega, John
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 1
  • DOI: 10.5194/acp-18-311-2018

Radiative forcing by long-lived greenhouse gases: Calculations with the AER radiative transfer models
journal, January 2008

  • Iacono, Michael J.; Delamere, Jennifer S.; Mlawer, Eli J.
  • Journal of Geophysical Research, Vol. 113, Issue D13
  • DOI: 10.1029/2008JD009944

A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
journal, January 2007

  • Petters, M. D.; Kreidenweis, S. M.
  • Atmospheric Chemistry and Physics, Vol. 7, Issue 8
  • DOI: 10.5194/acp-7-1961-2007

Sources and Secondary Production of Organic Aerosols in the Northeastern United States during WINTER
journal, July 2018

  • Schroder, J. C.; Campuzano-Jost, P.; Day, D. A.
  • Journal of Geophysical Research: Atmospheres
  • DOI: 10.1029/2018JD028475

Real-time aerosol mass spectrometry with millisecond resolution
journal, May 2011

  • Kimmel, Joel R.; Farmer, Delphine K.; Cubison, Michael J.
  • International Journal of Mass Spectrometry, Vol. 303, Issue 1
  • DOI: 10.1016/j.ijms.2010.12.004

MIX: a mosaic Asian anthropogenic emission inventory under the international collaboration framework of the MICS-Asia and HTAP
journal, January 2017

  • Li, Meng; Zhang, Qiang; Kurokawa, Jun-ichi
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 2
  • DOI: 10.5194/acp-17-935-2017

An updated climatology of surface dimethlysulfide concentrations and emission fluxes in the global ocean: UPDATED DMS CLIMATOLOGY
journal, January 2011

  • Lana, A.; Bell, T. G.; Simó, R.
  • Global Biogeochemical Cycles, Vol. 25, Issue 1
  • DOI: 10.1029/2010GB003850

Year-round record of bulk and size-segregated aerosol composition in central Antarctica (Concordia site) – Part 2: Biogenic sulfur (sulfate and methanesulfonate) aerosol
journal, January 2017

  • Legrand, Michel; Preunkert, Susanne; Weller, Rolf
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 22
  • DOI: 10.5194/acp-17-14055-2017

Atmospheric aerosol models for systems including the ions H + , NH 4 + , Na + , SO 4 2− , NO 3 − , Cl − , Br − , and H 2 O
journal, January 2002

Limitations in the enhancement of visible light absorption due to mixing state
journal, January 2006

  • Bond, Tami C.; Habib, Gazala; Bergstrom, Robert W.
  • Journal of Geophysical Research, Vol. 111, Issue D20
  • DOI: 10.1029/2006JD007315

New Particle Formation from Methanesulfonic Acid and Amines/Ammonia as a Function of Temperature
journal, December 2016

  • Chen, Haihan; Finlayson-Pitts, Barbara J.
  • Environmental Science & Technology, Vol. 51, Issue 1
  • DOI: 10.1021/acs.est.6b04173

Theoretical constraints on pure vapor-pressure driven condensation of organics to ultrafine particles: ORGANIC CONDENSATION
journal, August 2011

  • Donahue, N. M.; Trump, E. R.; Pierce, J. R.
  • Geophysical Research Letters, Vol. 38, Issue 16
  • DOI: 10.1029/2011GL048115

Chemical Transformation of Methanesulfonic Acid and Sodium Methanesulfonate through Heterogeneous OH Oxidation
journal, July 2018

Seasonality of sulfur species (dimethyl sulfide, sulfate, and methanesulfonate) in Antarctica: Inland versus coastal regions
journal, January 2008

  • Preunkert, Susanne; Jourdain, Bruno; Legrand, Michel
  • Journal of Geophysical Research, Vol. 113, Issue D15
  • DOI: 10.1029/2008JD009937

Methane sulfonic acid-enhanced formation of molecular clusters of sulfuric acid and dimethyl amine
journal, January 2014

Heterogeneous Oxidation of Particulate Methanesulfonic Acid by the Hydroxyl Radical: Kinetics and Atmospheric Implications
journal, December 2017

Gas-aerosol relationships of H 2 SO 4 , MSA, and OH: Observations in the coastal marine boundary layer at Mace Head, Ireland
journal, January 2002

Thermodynamic Models of Aqueous Solutions Containing Inorganic Electrolytes and Dicarboxylic Acids at 298.15 K. 1. The Acids as Nondissociating Components
journal, May 2006

  • Clegg, Simon L.; Seinfeld, John H.
  • The Journal of Physical Chemistry A, Vol. 110, Issue 17
  • DOI: 10.1021/jp056149k

H 2 SO 4 vapor pressure of sulfuric acid and ammonium sulfate solutions
journal, February 1997

  • Marti, James J.; Jefferson, Anne; Cai, Xiao Ping
  • Journal of Geophysical Research: Atmospheres, Vol. 102, Issue D3
  • DOI: 10.1029/96JD03064

Pollution and the planetary albedo
journal, December 1974

Predicting global aerosol size distributions in general circulation models
journal, January 2002

Formation and growth of nucleated particles into cloud condensation nuclei: model–measurement comparison
journal, January 2013

  • Westervelt, D. M.; Pierce, J. R.; Riipinen, I.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 15
  • DOI: 10.5194/acp-13-7645-2013

Oceanic phytoplankton, atmospheric sulphur, cloud albedo and climate
journal, April 1987

  • Charlson, Robert J.; Lovelock, James E.; Andreae, Meinrat O.
  • Nature, Vol. 326, Issue 6114
  • DOI: 10.1038/326655a0

Characterization of the South Atlantic marine boundary layer aerosol using an aerodyne aerosol mass spectrometer
journal, January 2008

  • Zorn, S. R.; Drewnick, F.; Schott, M.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 16
  • DOI: 10.5194/acp-8-4711-2008
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