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Abstract
Significant changes were observed in the sub-micron aerosol size distribution during a clean and a polluted Lagrangian study of marine boundary layer (MBL) aerosol and meteorological evolution during ACE-2. These changes were accompanied by significant alterations in boundary layer meteorology and structure. The clean case (LAG1) shows a reduction in the fine mode aerosol from 1050 cm-3 to 750 cm-3 and an increase in the accumulation mode concentration from 76 cm-3 to 162 cm-3 over 26 h. Dominant meteorological features during the same period comprised a reduction in boundary layer height from δ1500 m to δ800 m and an increase in the surface layer wind speed from 5 m s-1 to 15 m s-1. A detailed time-scale analysis, based upon measured data and including processes such as coagulation, condensation, deposition, chemical processing, sea-salt flux and entrainment, suggests that the dominant loss process for fine mode aerosol is coagulation, while the enhancement of accumulation mode aerosol can be almost totally ascribed to enhanced sea-salt aerosol flux into the reduced mixed layer volume. Aerosol size distributions from the polluted Lagrangian (LAG2) indicated little growth in particle diameter, and both fine and accumulation mode were observed to decrease in concentration from 2700 cm-3 to 1150 cm-3 and from 670 cm-3 to 430 cm-3 in 26 h, respectively. Dilution with cleaner free tropospheric air as the boundary layer height increased from δ500 m to >1000 m is suggested to be the primary factor relating to reduced aerosol concentrations in this case. To a smaller extent, coagulation and precipitation scavenging were calculated to be of some importance. For both Lagrangian case studies, meteorological changes, followed by physical aerosol-cloud interactions, appear to have the greatest influence on the MBL aerosol size distribution and number concentration over the given time-scale.
