Impact of cloud processes on aerosol particle properties: results from two ATR-42 flights in an extended stratocumulus cloud layer during the EUCAARI campaign (2008)

Abstract. Within the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project, the Meteo France research aircraft ATR-42 was operated from Rotterdam airport during May 2008, to perform scientific flights dedicated to the investigation of aerosol-cloud interactions. Therein, the objective of this study is to illustrate the impact of cloud processing on the aerosol particles physical and chemical properties. The presented results are retrieved from measurements during a double-flight mission from Rotterdam (Netherlands) to Newcastle (UK) and back 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 (V), below and above the stratocumulus cloud show strong differences. Firstly, measurements at constant altitude above the cloud layer show decreasing mass concentrations with decreasing horizontal distance (210–0 km) to the cloud layer by a factor up to 7, whereas below the cloud and by same means of distance, the mass concentrations merely decrease by a factor of 2 on average. Secondly, the averaged aerosol size distributions, observed above and below the cloud layer, are of bimodal character with pronounced minima between Aitken and accumulation mode which is potentially the consequence of cloud processing. Finally, the chemical composition of aerosol particles is strongly dependent on the location relative to the cloud layer (vicinity or below/above cloud). In general, the nitrate and organic fractions decrease with decreasing distance to the cloud, in the transit from cloud–free conditions towards the cloud boundaries. The decrease of nitrate and organic compounds ranges at a factor of three to ten, affecting sulfate and ammonium compounds to be increasingly abundant in the aerosol chemical composition while approaching the cloud layer. Finally, the chemical composition of non-refractory evaporated cloud droplets measured within the cloud shows increased fractions of nitrate and organics (with respect to concentrations found below clouds), but also large amounts of sulfate, thus, related to activation of particles, made up of soluble compounds.