Atmos. Chem. Phys. Discuss., 13, 14927-14975, 2013
© Author(s) 2013. This work is distributed
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Long-term observations of positive cluster ion concentration, sources and sinks at the high altitude site of the Puy de Dôme
C. Rose1, J. Boulon1, M. Hervo1, H. Holmgren1, E. Asmi2, M. Ramonet3, P. Laj4, and K. Sellegri1
1Laboratoire de Météorologie Physique CNRS, UMR6016, Observatoire de Physique du Globe de Clermont-Ferrand, Université Blaise Pascal, France
2Finnish Meteorological Institute, P.O. Box 503, 00101 Helsinki, Finland
3Laboratoire des Sciences du Climat et de l'Environnement, UMR Commissariat à l'Energie Atomique/CNRS 1592, Gif-sur-Yvette, France
4Laboratoire de Glaciologie et Géophysique de l'Environnement, CNRS UMR5183, Université Joseph Fourier Grenoble 1, Saint Martin d'Héres, France

Abstract. Cluster particles (0.8–1.9 nm) are key entities involved in nucleation and new particle formation processes in the atmosphere. Cluster ions were characterized in clear sky conditions at the Puy de Dôme station (1465 m a.s.l). The studied dataset spread over five years (February 2007–February 2012), which provided a unique chance to catch seasonal variations of cluster ion properties at high altitude. Statistical values of the cluster ion concentration and diameter are reported for both positive and negative polarities. Cluster ions were found to be ubiquitous at the Puy de Dôme and displayed an annual variation with lower concentrations in spring. Positive cluster ions were less numerous than negative ones but were larger in diameters. Negative cluster ion properties seemed insensitive to the occurrence of a new particle formation (NPF) event while positive cluster ions appeared to be significantly more numerous and larger on event days. The parameters of the balance equation for the positive cluster concentration are reported, separately for the different seasons and for the NPF event days and non-event days. The steady state assumption suggests that the ionization rate is balanced with two sinks which are the ion recombination and the attachment on aerosol particles, referred as "aerosol ion sink". The aerosol ion sink was found to be higher during the warm season and dominated the loss of ions. The positive ionization rates derived from the balance equation were well correlated with the ionization rates obtained from radon measurement, and they were on average higher in summer and fall compared to winter and spring. Neither the aerosol ion sink nor the ionization rate were found to be significantly different on event days compared to non-event days, and thus they were not able to explain the different positive cluster concentrations between event and non-event days. Hence, the excess of positive small ions on event days may derive from an additional source of ions coupled with the fact that the steady state was not verified on event days.

Citation: Rose, C., Boulon, J., Hervo, M., Holmgren, H., Asmi, E., Ramonet, M., Laj, P., and Sellegri, K.: Long-term observations of positive cluster ion concentration, sources and sinks at the high altitude site of the Puy de Dôme, Atmos. Chem. Phys. Discuss., 13, 14927-14975, doi:10.5194/acpd-13-14927-2013, 2013.
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