1Brookhaven National Laboratory, Upton, New York, USA
2Pacific Northwest National Laboratory, Richland, Washington, USA
3Aerodyne Research Inc., Billerica, Massachusetts, USA
4State University of New York, Albany, New York, USA
5Yonsei University, Seoul, 120749, South Korea
6University of Manchester, Manchester, M13 9PL, UK
Abstract. During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O3 and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate in agreement with the dominant pollution source being SO2 from Cu smelters and power plants. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 °C with dry air descending from the upper atmospheric and moist air having a BL contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (Dp > 100 nm) gives a linear relation up to a number concentration of ~150 cm−3, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that ~25 % of aerosol in the PCASP size range are interstitial (not activated). One hundred and two constant altitude cloud transects were identified and used to determine properties of interstitial aerosol. One transect is examined in detail as a case study. Approximately 25 to 50 % of aerosol with Dp > 110 nm were not activated, the difference between the two approaches possibly representing shattered cloud droplets or unknown artifact. CDNC and interstitial aerosol were anti-correlated in all cloud transects, consistent with the occurrence of dry in-cloud areas due to entrainment or circulation mixing.