Sensitivities of sulfate aerosol formation and oxidation pathways on the chemical mechanism employed in simulations

by A F Stein, R D Saylor
Atmospheric Chemistry and Physics ()


The processes of aerosol sulfate formation are vital components in the scientific understanding of perturbations of earth's radiative balance via aerosol direct and indirect effects. In this work, an analysis of the influence of changes in oxidant levels and sulfur dioxide oxidation pathways was performed to study the underlying pathways for sulfate formation. Sensitivities of this constituent were calculated from a series of photochemical model simulations with varying rates of NOx and VOC emissions to produce variations in oxidant abundances using a photochemical model (CMAQ) that covers the eastern US for part of the ICARTT 2004 campaign. Three different chemical mechanisms (CBIV, CB05, and SAPRC99) were used to test model responses to changes in NOx and VOC concentrations. Comparison of modeled results and measurements demonstrates that the simulations with all three chemical mechanisms capture the levels of sulfate reasonably well. However, the three mechanisms are shown to have significantly different responses in sulfate formation when the emissions of NOx and/or VOC are altered, reflecting different photochemical regimes under which the formation of sulfate occurs. Also, an analysis of the oxidation pathways that contribute to sulfur dioxide conversion to sulfate reveals substantial differences in the importance of the various pathways among the three chemical mechanisms. These findings suggest that estimations of the influence that future changes in primary emissions or other changes which perturb SO2 oxidants have on sulfate abundances, and on its direct and indirect radiative forcing effects, may be dependent on the chemical mechanism employed in the model analysis.

Cite this document (BETA)

Readership Statistics

10 Readers on Mendeley
by Discipline
by Academic Status
30% Ph.D. Student
30% Post Doc
10% Researcher (at a non-Academic Institution)
by Country
10% United States

Sign up today - FREE

Mendeley saves you time finding and organizing research. Learn more

  • All your research in one place
  • Add and import papers easily
  • Access it anywhere, anytime

Start using Mendeley in seconds!

Sign up & Download

Already have an account? Sign in