Articles | Volume 17, issue 14
Atmos. Chem. Phys., 17, 8887–8901, 2017
Atmos. Chem. Phys., 17, 8887–8901, 2017

Research article 24 Jul 2017

Research article | 24 Jul 2017

Modeling the role of highly oxidized multifunctional organic molecules for the growth of new particles over the boreal forest region

Emilie Öström1,2, Zhou Putian3, Guy Schurgers4, Mikhail Mishurov5, Niku Kivekäs6, Heikki Lihavainen6, Mikael Ehn3, Matti P. Rissanen3, Theo Kurtén7, Michael Boy3, Erik Swietlicki1, and Pontus Roldin1,3 Emilie Öström et al.
  • 1Division of Nuclear Physics, Lund University, Lund, P.O. Box 118, 221 00, Sweden
  • 2Centre for Environmental and Climate Research, Lund University, Lund, P.O. Box 118, 221 00, Sweden
  • 3Department of Physics, University of Helsinki, Helsinki, P.O. Box 64, 00014, Finland
  • 4Department of Geosciences and Natural Resource Management, University of Copenhagen, Copenhagen, 1350, Denmark
  • 5Department of Physical Geography and Ecosystem Science, Lund University, Lund, 223 62, Sweden
  • 6Finnish Meteorological Institute, Helsinki, P.O. Box 503, 00101, Finland
  • 7Department of Chemistry, University of Helsinki, Helsinki, P.O. Box 55, 00014, Finland

Abstract. In this study, the processes behind observed new particle formation (NPF) events and subsequent organic-dominated particle growth at the Pallas Atmosphere–Ecosystem Supersite in Northern Finland are explored with the one-dimensional column trajectory model ADCHEM. The modeled sub-micron particle mass is up to  ∼  75 % composed of SOA formed from highly oxidized multifunctional organic molecules (HOMs) with low or extremely low volatility. In the model the newly formed particles with an initial diameter of 1.5 nm reach a diameter of 7 nm about 2 h earlier than what is typically observed at the station. This is an indication that the model tends to overestimate the initial particle growth. In contrast, the modeled particle growth to CCN size ranges ( >  50 nm in diameter) seems to be underestimated because the increase in the concentration of particles above 50 nm in diameter typically occurs several hours later compared to the observations. Due to the high fraction of HOMs in the modeled particles, the oxygen-to-carbon (O  :  C) atomic ratio of the SOA is nearly 1. This unusually high O  :  C and the discrepancy between the modeled and observed particle growth might be explained by the fact that the model does not consider any particle-phase reactions involving semi-volatile organic compounds with relatively low O  :  C. In the model simulations where condensation of low-volatility and extremely low-volatility HOMs explain most of the SOA formation, the phase state of the SOA (assumed either liquid or amorphous solid) has an insignificant impact on the evolution of the particle number size distributions. However, the modeled particle growth rates are sensitive to the method used to estimate the vapor pressures of the HOMs. Future studies should evaluate how heterogeneous reactions involving semi-volatility HOMs and other less-oxidized organic compounds can influence the SOA composition- and size-dependent particle growth.

Short summary
We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Final-revised paper