1University of Hawaii at Manoa, Department of Oceanography, Honolulu, HI, USA
2University of California San Diego, Scripps Institute of Oceanography, La Jolla, CA, USA
3University of Washington, Department of Atmospheric Sciences, Seattle, WA, USA
4National Oceanographic and Atmospheric Administration, Pacific Marine Environmental Laboratory, Seattle, WA, USA
5Drexel University, Department of Chemistry, Philadelphia, PA, USA
6Oregon State University, College of Oceanic and Atmospheric Sciences, Corvallis, OR, USA
7University of Miami, Rosenstiel School of Marine and Atmospheric Science, Miami, FL, USA
8Ball Aerospace and Technologies, Corp., Boulder, CO, USA
9National Oceanographic and Atmospheric Administration, Earth System Research Laboratory, Boulder, CO, USA
10Colorado State University, Department of Atmospheric Science, Fort Collins, CO, USA
Received: 10 Jan 2011 – Discussion started: 24 Jan 2011
Abstract. 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−.
Revised: 20 May 2011 – Accepted: 24 May 2011 – Published: 31 May 2011
Yang, M., Huebert, B. J., Blomquist, B. W., Howell, S. G., Shank, L. M., McNaughton, C. S., Clarke, A. D., Hawkins, L. N., Russell, L. M., Covert, D. S., Coffman, D. J., Bates, T. S., Quinn, P. K., Zagorac, N., Bandy, A. R., de Szoeke, S. P., Zuidema, P. D., Tucker, S. C., Brewer, W. A., Benedict, K. B., and Collett, J. L.: Atmospheric sulfur cycling in the southeastern Pacific – longitudinal distribution, vertical profile, and diel variability observed during VOCALS-REx, Atmos. Chem. Phys., 11, 5079-5097, doi:10.5194/acp-11-5079-2011, 2011.