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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 30 Apr 2019

Research article | 30 Apr 2019

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

Seasonal characteristics of organic aerosol chemical composition and volatility in Stuttgart, Germany

Wei Huang1,2, Harald Saathoff1, Xiaoli Shen1,2, Ramakrishna Ramisetty1,a, Thomas Leisner1,3, and Claudia Mohr4 Wei Huang et al.
  • 1Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Eggenstein-Leopoldshafen, 76344, Germany
  • 2Institute of Geography and Geoecology, Working Group for Environmental Mineralogy and Environmental System Analysis, Karlsruhe Institute of Technology, Karlsruhe, 76131, Germany
  • 3Institute of Environmental Physics, Heidelberg University, Heidelberg, 69120, Germany
  • 4Department of Environmental Science and Analytical Chemistry, Stockholm University, Stockholm, 11418, Sweden
  • anow at: TSI Instruments India Private Limited, Bangalore, 560102, India

Abstract. Chemical composition and volatility of organic aerosol (OA) particles were investigated during July–August 2017 and February–March 2018 in the city of Stuttgart, one of the most polluted cities in Germany. Total non-refractory particle mass was measured with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS; hereafter AMS). Aerosol particles were collected on filters and analyzed in the laboratory with a filter inlet for gases and aerosols coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (FIGAERO-HR-ToF-CIMS; hereafter CIMS), yielding the molecular composition of oxygenated OA (OOA) compounds. While the average organic mass loadings are lower in the summer period (5.1 ± 3.2 µg m−3) than in the winter period (8.4 ± 5.6 µg m−3), we find relatively larger mass contributions of organics measured by AMS in summer (68.8 ± 13.4 %) compared to winter (34.8 ± 9.5 %). CIMS mass spectra show OOA compounds in summer have O : C ratios of 0.82 ± 0.02 and are more influenced by biogenic emissions, while OOA compounds in winter have O : C ratios of 0.89 ± 0.06 and are more influenced by biomass burning emissions. Volatility parametrization analysis shows that OOA in winter is less volatile with higher contributions of low volatile organic compounds (LVOC) and extremely low volatile organic compounds (ELVOC). We partially explain this by the higher contributions of compounds with shorter carbon chain lengths and higher number of oxygen atoms, i.e. higher O : C ratios in winter. Organic compounds desorbing from the particles deposited on the filter samples also exhibit a shift of signal to higher desorption temperatures (i.e. lower apparent volatility) in winter. This is consistent with the relatively higher O : C ratios in winter, but may also be related to higher particle viscosity due to the higher contributions of larger molecular-weight LVOC and ELVOC, interactions between different species and/or particles (particle matrix), and/or thermal decomposition of larger molecules. The results suggest that whereas lower temperature in winter may lead to increased partitioning of semi-volatile organic compounds (SVOC) into the particle phase, this does not result in a higher overall volatility of OOA in winter, and that the difference in sources and/or chemistry between the seasons plays a more important role. Our study provides insights into the seasonal variation of molecular composition and volatility of ambient OA particles, and into their potential sources.

Wei Huang et al.
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Short summary
We investigate molecular composition and volatility of oxygenated organic aerosol (OOA) particles in summer and winter in Stuttgart, Germany. OOA in summer is more influenced by biogenic emissions, while in winter biomass burning emissions are an important source. OOA in winter is also less volatile. Potential reasons are discussed in our manuscript. Our study shows the important contributions of non-fossil OA from biogenic and biomass burning even in an urban area with high traffic emissions.
We investigate molecular composition and volatility of oxygenated organic aerosol (OOA)...