Effect of sulfate aerosol on tropospheric NOx and ozone budgets

Model simulations and TOPSE evidence

Xuexi Tie, Louisa Emmons, Larry Horowitz, Guy Brasseur, Brian Ridley, Elliot L Atlas, Craig Stround, Peter Hess, Andrzej Klonecki, Sasha Madronich, Robert Talbot, Jack Dibb

Research output: Contribution to journalArticle

53 Citations (Scopus)

Abstract

The distributions of NOx and O3 are analyzed during TOPSE (Tropospheric Ozone Production about the Spring Equinox). In this study these data are compared with the calculations of a global chemical/transport model (Model for OZone And Related chemical Tracers (MOZART)). Specifically, the effect that hydrolysis of N2O5 on sulfate aerosols has on tropospheric NOx and O3 budgets is studied. The results show that without this heterogeneous reaction, the model significantly overestimates NOx concentrations at high latitudes of the Northern Hemisphere (NH) in winter and spring in comparison to the observations during TOPSE; with this reaction, modeled NOx concentrations are close to the measured values. This comparison provides evidence that the hydrolysis of N2O5 on sulfate aerosol plays an important role in controlling the tropospheric NOx and O3 budgets. The calculated reduction of NOx attributed to this reaction is 80 to 90% in winter at high latitudes over North America. Because of the reduction of NOx, O3 concentrations are also decreased. The maximum O3 reduction occurs in spring although the maximum NOx reduction occurs in winter when photochemical O3 production is relatively low. The uncertainties related to uptake coefficient and aerosol loading in the model is analyzed. The analysis indicates that the changes in NOx due to these uncertainties are much smaller than the impact of hydrolysis of N2O5 on sulfate aerosol. The effect that hydrolysis of N2O5 on global NOx and O3 budgets are also assessed by the model. The results suggest that in the Northern Hemisphere, the average NOx budget decreases 50% due to this reaction in winter and 5% in summer. The average O3 budget is reduced by 8% in winter and 6% in summer. In the Southern Hemisphere (SH), the sulfate aerosol loading is significantly smaller than in the Northern Hemisphere. As a result, sulfate aerosol has little impact on NOx and O3 budgets of the Southern Hemisphere.

Original languageEnglish (US)
Pages (from-to)12-11
Number of pages2
JournalJournal of Geophysical Research C: Oceans
Volume108
Issue number4
StatePublished - Feb 27 2003
Externally publishedYes

Fingerprint

Ozone
Aerosols
budgets
Sulfates
ozone
sulfates
aerosols
winter
aerosol
sulfate
hydrolysis
Hydrolysis
Northern Hemisphere
simulation
Southern Hemisphere
polar regions
summer
tracers
budget
effect

Keywords

  • NO
  • Ozone
  • Tropospheric aerosol

ASJC Scopus subject areas

  • Earth and Planetary Sciences (miscellaneous)
  • Atmospheric Science
  • Geochemistry and Petrology
  • Geophysics
  • Oceanography
  • Space and Planetary Science
  • Astronomy and Astrophysics

Cite this

Effect of sulfate aerosol on tropospheric NOx and ozone budgets : Model simulations and TOPSE evidence. / Tie, Xuexi; Emmons, Louisa; Horowitz, Larry; Brasseur, Guy; Ridley, Brian; Atlas, Elliot L; Stround, Craig; Hess, Peter; Klonecki, Andrzej; Madronich, Sasha; Talbot, Robert; Dibb, Jack.

In: Journal of Geophysical Research C: Oceans, Vol. 108, No. 4, 27.02.2003, p. 12-11.

Research output: Contribution to journalArticle

Tie, X, Emmons, L, Horowitz, L, Brasseur, G, Ridley, B, Atlas, EL, Stround, C, Hess, P, Klonecki, A, Madronich, S, Talbot, R & Dibb, J 2003, 'Effect of sulfate aerosol on tropospheric NOx and ozone budgets: Model simulations and TOPSE evidence', Journal of Geophysical Research C: Oceans, vol. 108, no. 4, pp. 12-11.
Tie, Xuexi ; Emmons, Louisa ; Horowitz, Larry ; Brasseur, Guy ; Ridley, Brian ; Atlas, Elliot L ; Stround, Craig ; Hess, Peter ; Klonecki, Andrzej ; Madronich, Sasha ; Talbot, Robert ; Dibb, Jack. / Effect of sulfate aerosol on tropospheric NOx and ozone budgets : Model simulations and TOPSE evidence. In: Journal of Geophysical Research C: Oceans. 2003 ; Vol. 108, No. 4. pp. 12-11.
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abstract = "The distributions of NOx and O3 are analyzed during TOPSE (Tropospheric Ozone Production about the Spring Equinox). In this study these data are compared with the calculations of a global chemical/transport model (Model for OZone And Related chemical Tracers (MOZART)). Specifically, the effect that hydrolysis of N2O5 on sulfate aerosols has on tropospheric NOx and O3 budgets is studied. The results show that without this heterogeneous reaction, the model significantly overestimates NOx concentrations at high latitudes of the Northern Hemisphere (NH) in winter and spring in comparison to the observations during TOPSE; with this reaction, modeled NOx concentrations are close to the measured values. This comparison provides evidence that the hydrolysis of N2O5 on sulfate aerosol plays an important role in controlling the tropospheric NOx and O3 budgets. The calculated reduction of NOx attributed to this reaction is 80 to 90{\%} in winter at high latitudes over North America. Because of the reduction of NOx, O3 concentrations are also decreased. The maximum O3 reduction occurs in spring although the maximum NOx reduction occurs in winter when photochemical O3 production is relatively low. The uncertainties related to uptake coefficient and aerosol loading in the model is analyzed. The analysis indicates that the changes in NOx due to these uncertainties are much smaller than the impact of hydrolysis of N2O5 on sulfate aerosol. The effect that hydrolysis of N2O5 on global NOx and O3 budgets are also assessed by the model. The results suggest that in the Northern Hemisphere, the average NOx budget decreases 50{\%} due to this reaction in winter and 5{\%} in summer. The average O3 budget is reduced by 8{\%} in winter and 6{\%} in summer. In the Southern Hemisphere (SH), the sulfate aerosol loading is significantly smaller than in the Northern Hemisphere. As a result, sulfate aerosol has little impact on NOx and O3 budgets of the Southern Hemisphere.",
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AU - Hess, Peter

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