Airborne investigation of the aerosols–cloud interactions in the vicinity and within a marine stratocumulus over the North Sea during EUCAARI (2008)

Within the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project, the Meteo France research aircraft ATR-42 was operated from Rotterdam (Netherlands) airport during May 2008, to perform scientific flights dedicated to the investigation of aerosol–cloud interactions. The objective of this study is to illustrate the impact of cloud processing on the aerosol particle physical and chemical properties. The presented results are retrieved from measurements during flight operation with two consecutive flights, first from Rotterdam to Newcastle (United Kingdom) and subsequently reverse along the same waypoints back to Rotterdam using data measured with compact Time of Flight Aerosol Mass Spectrometer (cToF-AMS) and Scanning Mobility Particle Sizer (SMPS). Cloud-related measurements during these flights were performed over the North Sea within as well as in close vicinity of a marine stratocumulus cloud layer. Particle physical and chemical properties observed in the close vicinity, below and above the stratocumulus cloud, show strong differences: (1) the averaged aerosol size distributions, observed above and below the cloud layer, are of bimodal character with pronounced minima between Aitken and accumulation mode, very likely due to cloud processing. (2) the chemical composition of aerosol particles is strongly dependent on the position relative to the cloud layer (vicinity or below/above cloud). In general, the nitrate and organic relative mass fractions decrease with decreasing distance to the cloud, in the transit from cloud–free conditions towards the cloud boundaries. This relative mass fraction decrease ranges from a factor of three to ten, thus leading to an increase of the sulfate and ammonium relative mass concentrations while approaching the cloud layer. (3), the chemical composition of cloud droplet residuals, analyzed downstream of a Counterflow virtual Impactor (CVI) inlet indicates increased fractions of mainly soluble chemical compounds such as nitrate and organics, compared to non cloud processed particles. Finally, a net overbalance of nitrate aerosol has been revealed by comparing cloud droplet residual and non cloud processed aerosol chemical compositions. Conclusively, this study highlights gaps concerning the sampling strategy that need to be addressed for the future missions.