Modeling and measurements of Modeling and measurements of oxygen isotope tracers of oxygen isotope tracers of sulfate formation: sulfate formation: Implications for the sulfur Implications for the sulfur budget in the marine boundary budget in the marine boundary layer layer Becky Alexander, Rokjin Park, Daniel J. Jacob, Robert M. Yantosca Harvard University, Department of Earth and Planetary Sciences Joël Savarino, Charles. C.W. Lee, Mark H. Thiemens University of California, San Diego, Department of Chemistry and Biochemsitry Mian Chin NASA Goddard Space Flight Center AGU, Fall 2003
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Modeling and measurements of oxygen isotope tracers of sulfate formation: Implications for the sulfur budget in the marine boundary layer Becky Alexander,
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Modeling and measurements of Modeling and measurements of oxygen isotope tracers of sulfate oxygen isotope tracers of sulfate
formation: Implications for the sulfur formation: Implications for the sulfur budget in the marine boundary layerbudget in the marine boundary layer
Becky Alexander, Rokjin Park, Daniel J. Jacob, Robert M. Yantosca
Harvard University, Department of Earth and Planetary Sciences
Joël Savarino, Charles. C.W. Lee, Mark H. Thiemens
University of California, San Diego, Department of Chemistry and Biochemsitry
Percent (%) change in concentrations (yearly average)
Case A: SO2/SO42- concentration without sea-salt chemistry
Case B: With sea-salt chemistry
SO2 (decrease) SO42- (small increase)
|100|
CaseA
CaseBCaseA
Effect of sea-salt chemistry on SOEffect of sea-salt chemistry on SO22 and and
SOSO442-2- concentrations concentrations
50%0% 100%
Effect of sea-salt chemistry on gas-phase Effect of sea-salt chemistry on gas-phase sulfate production ratessulfate production rates
|100|
CaseA
CaseBCaseA
Mar/Apr/May Jun/Jul/Aug
Sep/Oct/Nov Dec/Jan/Feb
Percent (%) decrease (seasonal average):
Aqueous versus Gas Phase OxidationAqueous versus Gas Phase Oxidation
Biological regulation of the climate?
(Charlson et al., 1987)
DMSOH
NO3 SO2 H2SO4OH
New particle formation
CCN
H2O2
Light scattering
Gas-phaseAqueous-phase
Aqueous-phase
O3
ConclusionsConclusions
•Sulfate17O provides information on relative oxidation pathways (gas OH versus aqueous O3,H2O2) in the atmosphere
•Measurements from INDOEX show that O3 oxidation is an important mechanism for sulfate formation over the ocean
•The magnitude and trend of 17O sulfate can be represented in the GEOS-CHEM model only with the addition of chemical formation in sea-salt aerosols
•Sulfate17O measurements provide an additional constraint for chemical transport models improve our understanding of sulfur chemistry and the sulfur budget