References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-11589-2012

Aerosol cloud activation in summer and winter at puy-de-Dôme high altitude site in France

Asmi

¹ ² Freney

¹ Hervo

¹ Picard

¹ Rose

¹ Colomb

¹ Sellegri

Laboratoire de Météorologie Physique, UMR6016, Université Blaise Pascal, Clermont-Ferrand, France

now at: Finnish Meteorological Institute, Erik Palménin aukio 1, 00560 Helsinki, Finland

04 12 2012

12 23 11589 11607

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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Cloud condensation nuclei (CCN) size distributions and numbers were measured for the first time at Puy-de-Dôme high altitude (1465 m a.s.l) site in Central France. Majority of the measurements were done at constant supersaturation (SS) of 0.24%, which was also deduced to be representative of the typical in-cloud SS at the site. CCN numbers during summer ranged from about 200 up to 2000 cm−3 and during winter from 50 up to 3000 cm−3. Variability of CCN number was explained by both particle chemistry and size distribution variability. The higher CCN concentrations were measured in continental, in contrast to marine, air masses. Aerosol CCN activity was described with a single hygroscopicity parameter κ. Range of this parameter was 0.29 ± 0.13 in summer and 0.43 ± 0.19 in winter. When calculated using SS of 0.51% during summer, κ of 0.22 ± 0.07 was obtained. The decrease with increasing SS is likely explained by the particle size dependent chemistry with smaller particles containing higher amounts of freshly emitted organic species. Higher κ values during winter were for the most part explained by the observed aged organics (analysed from organic m/z 44 ratio) rather than from aerosol organic to inorganic volume fraction. The obtained κ values also fit well within the range of previously proposed global continental κ of 0.27 ± 0.21. During winter, the smallest κ values and the highest organic fractions were measured in marine air masses. CCN closure using bulk AMS chemistry led to positive bias of 5% and 2% in winter and summer, respectively. This is suspected to stem from size dependent aerosol organic fraction, which is underestimated by using AMS bulk mass composition. Finally, the results were combined with size distributions measured from interstitial and whole air inlets to obtain activated droplet size distributions. Cloud droplet number concentrations were shown to increase with accumulation mode particle number, while the real in-cloud SS correspondingly decreased. These results provide evidence on the effects of aerosol particles on maximum cloud supersaturations. Further work with detailed characterisation of cloud properties is proposed in order to provide more quantitative estimates on aerosol effects on clouds.

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