Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes

The response of marine low cloud systems to changes in aerosol concentration represents one of the largest uncertainties in climate simulations. Major contributions to this uncertainty are derived from poor understanding of aerosol under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse marine boundary layer (MBL) clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In this study, we examine MBL aerosol properties, trace gas mixing ratios, and meteorological parameters measured at the Atmospheric Radiation Measurement Climate Research Facility's ENA site on Graciosa Island, Azores, Portugal, during a 3-year period from 2015 to 2017. Measurements impacted by local pollution on Graciosa Island and during occasional intense biomass burning and dust events are excluded from this study. Submicron aerosol size distribution typically consists of three modes: Aitken (At, diameter D-p <similar to 100 nm), accumulation (Ac, D-p within similar to 100 to similar to 300 nm), and larger accumulation (LA, D-p >similar to 300 nm) modes, with average number concentrations (denoted as N-At, N-Ac, and N-LA below) of 330, 114, and 14 cm(-3), respectively. N-At, N-Ac, and N-LA show contrasting seasonal variations, suggesting different sources and removal processes. N-LA is dominated by sea spray aerosol (SSA) and is higher in winter and lower in summer. This is due to the seasonal variations of SSA production, in- cloud coalescence scavenging, and dilution by entrained free troposphere (FT) air. In comparison, SSA typically contributes a relatively minor fraction to N-At (10 %) and N-Ac (21 %) on an annual basis. In addition to SSA, sources of Acmode particles include entrainment of FT aerosols and condensation growth of Aitken-mode particles inside the MBL, while in-cloud coalescence scavenging is the major sink of N-Ac. The observed seasonal variation of N-Ac, being higher in summer and lower in winter, generally agrees with the steady-state concentration estimated from major sources and sinks. N-At is mainly controlled by entrainment of FT aerosol, coagulation loss, and growth of Aitken-mode particles into the Ac-mode size range. Our calculation suggests that besides the direct contribution from entrained FT Ac-mode particles, growth of entrained FT Aitken-mode particles in the MBL also represent a substantial source of cloud condensation nuclei (CCN), with the highest contribution potentially reaching 60% during summer. The growth of Aitken-mode particles to CCN size is an expected result of the condensation of sulfuric acid, a product from dimethyl sulfide oxidation, suggesting that ocean ecosystems may have a substantial influence on MBL CCN populations in the ENA.