References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-5079-2011

Atmospheric sulfur cycling in the southeastern Pacific – longitudinal distribution, vertical profile, and diel variability observed during VOCALS-REx

Yang

¹ Huebert

B. J.

¹ Blomquist

B. W.

¹ Howell

S. G.

¹ Shank

L. M.

¹ McNaughton

C. S.

¹ Clarke

A. D.

¹ Hawkins

L. N.

² Russell

L. M.

² Covert

D. S.

³ Coffman

D. J.

⁴ Bates

T. S.

⁴ Quinn

P. K.

⁴ Zagorac

⁵ Bandy

A. R.

⁵ de Szoeke

S. P.

⁶ Zuidema

P. D.

⁷ Tucker

S. C.

⁸ Brewer

W. A.

⁹ Benedict

K. B.

¹⁰ Collett

J. L.

¹⁰

University of Hawaii at Manoa, Department of Oceanography, Honolulu, HI, USA

University of California San Diego, Scripps Institute of Oceanography, La Jolla, CA, USA

University of Washington, Department of Atmospheric Sciences, Seattle, WA, USA

National Oceanographic and Atmospheric Administration, Pacific Marine Environmental Laboratory, Seattle, WA, USA

Drexel University, Department of Chemistry, Philadelphia, PA, USA

Oregon State University, College of Oceanic and Atmospheric Sciences, Corvallis, OR, USA

University of Miami, Rosenstiel School of Marine and Atmospheric Science, Miami, FL, USA

Ball Aerospace and Technologies, Corp., Boulder, CO, USA

National Oceanographic and Atmospheric Administration, Earth System Research Laboratory, Boulder, CO, USA

Colorado State University, Department of Atmospheric Science, Fort Collins, CO, USA

31 05 2011

11 10 5079 5097

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Dimethylsulfide (DMS) emitted from the ocean is a biogenic precursor gas for sulfur dioxide (SO2) and non-sea-salt sulfate aerosols (SO42−). During the VAMOS-Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) in 2008, multiple instrumented platforms were deployed in the Southeastern Pacific (SEP) off the coast of Chile and Peru to study the linkage between aerosols and stratocumulus clouds. We present here observations from the NOAA Ship Ronald H. Brown and the NSF/NCAR C-130 aircraft along ~20° S from the coast (70° W) to a remote marine atmosphere (85° W). While SO42− and SO2 concentrations were distinctly elevated above background levels in the coastal marine boundary layer (MBL) due to anthropogenic influence (~800 and 80 pptv, respectively), their concentrations rapidly decreased west of 78° W (~100 and 25 pptv). In the remote region, entrainment from the free troposphere (FT) increased MBL SO2 burden at a rate of 0.05 ± 0.02 μmoles m−2 day−1 and diluted MBL SO42 burden at a rate of 0.5 ± 0.3 μmoles m−2 day−1, while the sea-to-air DMS flux (3.8 ± 0.4 μmoles m−2 day−1) remained the predominant source of sulfur mass to the MBL. In-cloud oxidation was found to be the most important mechanism for SO2 removal and in situ SO42− production. Surface SO42− concentration in the remote MBL displayed pronounced diel variability, increasing rapidly in the first few hours after sunset and decaying for the rest of the day. We theorize that the increase in SO42− was due to nighttime recoupling of the MBL that mixed down cloud-processed air, while decoupling and sporadic precipitation scavenging were responsible for the daytime decline in SO42−.

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