Articles | Volume 15, issue 6
Atmos. Chem. Phys., 15, 3413–3428, 2015
Atmos. Chem. Phys., 15, 3413–3428, 2015

Research article 27 Mar 2015

Research article | 27 Mar 2015

Major contribution of neutral clusters to new particle formation at the interface between the boundary layer and the free troposphere

C. Rose1, K. Sellegri1, E. Asmi2, M. Hervo1, E. Freney1, A. Colomb1, H. Junninen3, J. Duplissy3, M. Sipilä3, J. Kontkanen3, K. Lehtipalo3,4, and M. Kulmala3 C. Rose et al.
  • 1Laboratoire de Météorologie Physique CNRS UMR6016, Observatoire de Physique du Globe de Clermont-Ferrand, Université Blaise Pascal, Clermont-Ferrand, France
  • 2Finnish Meteorological Institute, P.O. Box 503, 00101 Helsinki, Finland
  • 3Department of Physics, University of Helsinki, Helsinki, Finland
  • 4Airmodus Ltd, Gutaf Hällströmin katu 2, 00560 Helsinki, Finland

Abstract. The formation of new aerosol particles in the atmosphere is a key process influencing the aerosol number concentration as well as the climate, in particular at high altitude, where the newly formed particles directly influence cloud formation. However, free tropospheric new particle formation (NPF) is poorly documented due to logistic limitations and complex atmospheric dynamics around high-altitude stations that make the observation of this day-time process challenging. Recent improvements in measurement techniques make now possible the detection of neutral clusters down to ~ 1 nm sizes, which opens new horizons in our understanding of the nucleation process. Indeed, only the charged fraction of clusters has been reported in the upper troposphere up to now. Here we report day-time concentrations of charged and neutral clusters (1 to 2.5 nm mobility diameter) recorded at the interface between the boundary layer (BL) and the FT as well as in the FT at the altitude site of Puy de Dôme (1465 m a.s.l.), central France, between 10 and 29 February 2012. Our findings demonstrate that in the FT, and especially at the interface between the BL and the FT, the formation of 1.5 nm neutral clusters significantly exceeds the one of ionic clusters during NPF events, clearly indicating that they dominate in the nucleation process. We also observe that the total cluster concentration significantly increases during NPF events compared to the other days, which was not clearly observed for the charged cluster population in the past. During the studied period, the nucleation process does not seem to be sulfuric acid-limited and could be promoted by the transport of pollutants to the upper troposphere, coupled with low temperatures.

Final-revised paper