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Discussion papers
https://doi.org/10.5194/acp-2018-1305
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1305
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 02 Jan 2019

Research article | 02 Jan 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Insights into the O : C dependent mechanisms controlling the evaporation of α-pinene secondary organic aerosol particles

Angela Buchholz1, Andrew T. Lambe2, Arttu Ylisirniö1, Zijun Li1, Olli-Pekka Tikkanen1, Celia Faiola3, Eetu Kari1, Liqing Hao1, Olli Luoma1, Wei Huang4, Claudia Mohr5, Douglas R. Worsnop1,2, Sergey A. Nizkorodov6, Taina Yli-Juuti1, Siegfried Schobesberger1, and Annele Virtanen1 Angela Buchholz et al.
  • 1Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
  • 2Aerodyne Research Inc., Billerica, MA 08121-3976, USA
  • 3Department of Ecology and Evolutionary Biology, University of California, Irvine, CA, USA
  • 4Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
  • 5Department of Environmental Science and Analytical Chemistry, Stockholm University, Stockholm, Sweden
  • 6Department of Chemistry, University of California, Irvine, CA, USA

Abstract. The volatility of oxidation products of volatile organic compounds (VOCs) in the atmosphere is a key factor to determine if they partition into the particle phase contributing to secondary organic aerosol (SOA) mass. Thus, linking volatility and measured particle composition will provide insights into SOA formation and its fate in the atmosphere. We produced a-pinene SOA with three different oxidation levels (characterised by average oxygen to carbon ratio, O:C=0.53, 0.69, and 0.96) in an oxidation flow reactor. We investigated the particle volatility by isothermal evaporation in clean air as a function of relative humidity (RH<2%, 40%, and 80%) and used a filter-based thermal desorption method to gain volatility and chemical composition information. We observed reduced particle evaporation for particles with increasing O:C ratio, indicating that particles become more resilient to evaporation with oxidative aging. Particle evaporation was increased in the presence of water vapour and presumably particulate water, at the same time the resistance of the residual particles to thermal desorption was increased as well. For SOA with O:C=0.96, the unexpectedly large increase of mean thermal desorption temperature and changes in the thermogram shapes under wet conditions (80% RH) were an indication of aqueous phase chemistry. For the lower O:C cases, some water induced composition changes were observed. However, the enhanced evaporation under wet conditions could be explained by the reduction of particle viscosity from the semi-solid to liquid-like range and the observed higher desorption temperature of the residual particles is a direct consequence of the increased removal of high volatility and remaining of low volatility compounds.

Angela Buchholz et al.
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Angela Buchholz et al.
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Short summary
We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to...
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