Contrasting Cloud Composition Between Coupled and Decoupled Marine Boundary Layer Clouds

Marine stratocumulus clouds often become decoupled from the vertical layer immediately above the ocean surface. This study contrasts cloud chemical composition between coupled and decoupled marine stratocumulus clouds. Cloud water and droplet residual particle composition were measured in clouds off the California coast during three airborne experiments in July-August of separate years (E-PEACE 2011, NiCE 2013, BOAS 2015). Decoupled clouds exhibited significantly lower overall mass concentrations in both cloud water and droplet residual particles, consistent with reduced cloud droplet number concentration and sub-cloud aerosol (Dp > 100 nm) number concentration, owing to detachment from surface sources. Non-refractory sub-micrometer aerosol measurements show that coupled clouds exhibit higher sulfate mass fractions in droplet residual particles, owing to more abundant precursor emissions from the ocean and ships. Consequently, decoupled clouds exhibited higher mass fractions of organics, nitrate, and ammonium in droplet residual particles, owing to effects of long-range transport from more distant sources. Total cloud water mass concentration in coupled clouds was dominated by sodium and chloride, and their mass fractions and concentrations exceeded those in decoupled clouds. Conversely, with the exception of sea salt constituents (e.g., Cl, Na, Mg, K), cloud water mass fractions of all species examined were higher in decoupled clouds relative to coupled clouds. These results suggest that an important variable is the extent to which clouds are coupled to the surface layer when interpreting microphysical data relevant to clouds and aerosol particles.