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Discussion papers | Copyright
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 12 Jan 2018

Research article | 12 Jan 2018

Review status
This discussion paper is a preprint. A revision of the manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP).

Simulating secondary organic aerosol from anthropogenic and biogenic precursors: comparison to outdoor chamber experiments, effect of oligomerization on SOA formation and reactive uptake of aldehydes

Florian Couvidat1, Marta G. Vivanco2, and Bertrand Bessagnet1 Florian Couvidat et al.
  • 1Institut National de l’Environnement Industriel et des Risques, Verneuil-en-Halatte, France
  • 2Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas (CIEMAT), Departamento de Medio Ambiente, Av. Complutense 40, 28040-Madrid, Spain

Abstract. New parameterizations for the formation of organic aerosols have been developed. These parameterizations cover SOA formation from biogenic and anthropogenic precursors, NOx dependency, oligomerization and the reactive uptake of pinonaldehyde. Those parameterizations are based on available experimental results.

The effects of those parameterizations are tested against various experiments carried out in previous studies inside the outdoor chamber Euphore. Two datasets of experiments were used: the anthropogenic experiments (were SOA is formed mainly from a mixture of toluene, 1,3,5-trimethylbenzene and o-xylene) and the biogenic experiments (were SOA is formed mainly from α-pinene and limonene). SOA formation inside the chamber is simulated by using the Secondary Organic Aerosol Processor (SOAP) model to take into account the dynamic evolution of concentrations.

When assuming no wall deposition of organic vapors, satisfactory results were obtained for the biogenic experiments and most of the anthropogenic experiments. However, the anthropogenic experiments seem to indicate a complex NOx dependency that could not be reproduced by the model. Oligomerization was found to have a strong effect on SOA composition and could have a strong effect on the formation of SOA. The uptake of pinonaldehyde (which is a high volatility SVOC) onto acidic aerosol was found to be too slow to occur under atmospheric conditions but less volatile or more reactive aldehydes could react in acidic aerosols indicating that the parameterization of Pun and Seigneur (2007) used in some air quality models may lead to an overestimation of SOA concentrations.

However, taking into account wall deposition of organic vapors (with the parameters of Zhang et al. (2014)) leads to a strong underestimation of SOA concentrations. This feature is consistent with the fact that the SOA mechanisms are based on environmental chamber data. This underestimation could however be corrected by decreasing the volatility of SVOC by a factor 3.

The effect of particle viscosity was also estimated. Low changes in concentrations were found when taking into account SOA viscosity. Taking it into account leads to a decrease of SVOC evaporation and prevents changes in concentration due to changes of temperature during the experiments.

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Short summary
Several new parameterizations and mechanisms for SOA formation are developed based on available experimental results. To evaluate the parameterizations, a box model was developped to simulate SOA formation from monoterpenes and aromatics in the environmental chamber Euphore. This box model takes into account oligomerization, non-ideality of the aerosol, multi-phase partitioning, aging, vapor wall losses, particle-phase diffusion. All this phenomena are rarely taken into account together.
Several new parameterizations and mechanisms for SOA formation are developed based on available...