1Institute of Geophysics, University of Hamburg, KlimaCampus, Hamburg, Germany
2Laboratoire de Météorologie Physique, CNRS, Université Blaise Pascal Aubière, France
Received: 28 Aug 2013 – Discussion started: 15 Oct 2013
Abstract. Until recently secondary organic carbon aerosol (SOA) mass concentrations have been systematically underestimated by three-dimensional atmospheric-chemistry-aerosol models. With a newly proposed concept of aging of organic vapours, more realistic model results for organic carbon aerosol mass concentrations can be achieved. Applying a mixed thermodynamic-kinetic approach for SOA formation shifted the aerosol size distribution towards particles in the cloud condensation nuclei size range, thereby emphasising the importance of SOA formation schemes for modelling realistic cloud and precipitation formation. The additional importance of hetero-molecular nucleation between H2SO4 and organic vapours remains to be evaluated in three-dimensional atmospheric-chemistry-aerosol models. Here a case study is presented focusing on Puy-de-Dôme, France in June 2010. The measurements indicate a considerable increase in SOA mass concentration during the measurement campaign, which could be reproduced by modelling using a simplified thermodynamic-kinetic approach for SOA formation and increased biogenic volatile organic compound (VOC) precursor emissions. Comparison with a thermodynamic SOA formation approach shows a huge improvement in modelled SOA mass concentration with the thermodynamic-kinetic approach for SOA formation. SOA mass concentration increases by a factor of up to 6 accompanied by a slight improvement of modelled particle size distribution. Even though nucleation events at Puy-de-Dôme were rare during the chosen period of investigation, a weak event in the boundary layer could be reproduced by the model in a sensitivity study when nucleation of low-volatile secondary organic vapour is included. Differences in the model results with and without nucleation of organic vapour are visible in the lower free troposphere over several days. Taking into account the nucleation of organic vapour leads to an increase in accumulation mode particles due to coagulation and condensational growth of nucleation and Aitken mode particles.
Revised: 18 Mar 2014 – Accepted: 19 Mar 2014 – Published: 16 Apr 2014
Langmann, B., Sellegri, K., and Freney, E.: Secondary organic aerosol formation during June 2010 in Central Europe: measurements and modelling studies with a mixed thermodynamic-kinetic approach, Atmos. Chem. Phys., 14, 3831-3842, doi:10.5194/acp-14-3831-2014, 2014.