Hygroscopic Growth of Atmospheric Aerosol Particles and Its Relation to Nucleation Scavenging in Clouds

University dissertation from Division of Nuclear Physics, Lund University, Box 118, S-221 00 Lund, Sweden

Abstract: Aerosol particles in the atmosphere are important in several aspects. Some major aerosol constituents that are deposited in ecosystems are acidic or fertilisers and some minor or trace constituents are toxic. Aerosol particles are also involved in the earth’s radiation balance, both directly by scattering the sunlight and indirectly by influencing the clouds. All these effects are influenced by the interaction between the aerosol particles and water vapour. A tandem differential mobility analyser (TDMA) has been designed to measure hygroscopic growth, i. e. the particle diameter change due to uptake of water at well defined relative humidities below 100 %. Tests of the instrument performance have been made using aerosol particles of pure inorganic salts. Three field experiments have been performed as parts of large fog and cloud experiments. Bimodal hygroscopic growth spectra were found: less-hygroscopic particles containing a few percent and more-hygroscopic particles around 50 % by volume of hygroscopically active material. In general the fraction of less-hygroscopic particles decreases with particle size and it is larger in polluted continental aerosols than in remote background aerosols. This external mixing cannot be fully understood using present views on the formation of aerosols. Evidence for the importance of the external mixing on the cloud nucleating properties of the particles are found in comparisons between hygroscopic growth spectra for the total aerosol, the interstitial aerosol in clouds, and cloud drop residuals. Cloud condensation nuclei spectra, calculated using aerosol particle size distributions and hygroscopic growth spectra, in combination with information on the major inorganic ions are presented. These CCN spectra reveal for instance that the influence of less-hygroscopic particles on the cloud droplets increases with increasing peak supersaturation. The fraction of the particles that were scavenged to cloud drops, as a function of particle size, are presented. A comparison between these result and cloud modelling, using detailed aerosol input, based on particle size distributions and hygroscopically active fractions determined from TDMA data showed good agreement.

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