Differentiating sulfate aerosol oxidation pathways for varying source altitudes using 35 S and Δ 17 O tracers

Due to the complex nature of the sulfur cycle, uncertainties remain in the transport rate and chemical transformation mechanisms of sulfur species, including sulfate aerosols. Here, we report oxygen isotopic anomaly and radioactive 35 S measurements in sulfate aerosols collected at La Jolla, Califor...

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Veröffentlicht in:Journal of Geophysical Research: Atmospheres 2012-09, Vol.117 (D18)
Hauptverfasser: Hill‐Falkenthal, Jason, Priyadarshi, Antra, Thiemens, Mark
Format: Artikel
Sprache:eng
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Zusammenfassung:Due to the complex nature of the sulfur cycle, uncertainties remain in the transport rate and chemical transformation mechanisms of sulfur species, including sulfate aerosols. Here, we report oxygen isotopic anomaly and radioactive 35 S measurements in sulfate aerosols collected at La Jolla, California during 2009–2010. A strong correlation results from increased levels of specific activity (up to 195 atoms of 35 S/nmol non sea salt (nss)‐SO 4 ) and Δ 17 O (up to 1.50‰) in sulfate aerosol (fine fraction) samples during Santa Ana wind events compared to background levels. This is possibly due to an increase in mixing of free tropospheric air mass, containing higher levels of 35 S specific activity and higher Δ 17 O, into the boundary layer. These tracers show the ability to detect changes in oxidation chemistry during high altitude air mixing events and have the potential to trace the changes in oxidation pathways of sulfur species during Stratospheric‐Tropospheric exchange events. Sampling at higher latitudes where deep stratospheric intrusions are more prominent can help further parameterize how stratosphere‐troposphere exchange events (STE) affect oxidation chemistry in the boundary layer. Santa Ana events show increased levels of both 35S and Delta17O Free tropospheric air mass mixing increases during Santa Ana events These tracers can be used to trace changes in oxidation due to STE
ISSN:0148-0227
DOI:10.1029/2012JD018242