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

<p><strong>Abstract.</strong> The 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 mea...

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Hauptverfasser: Huang, Wei (VerfasserIn) , Leisner, Thomas (VerfasserIn)
Dokumenttyp: Article (Journal)
Sprache:Englisch
Veröffentlicht: 19 September 2019
In: Atmospheric chemistry and physics
Year: 2019, Jahrgang: 19, Heft: 18, Pages: 11687-11700
ISSN:1680-7324
DOI:https://doi.org/10.5194/acp-19-11687-2019
Online-Zugang:Verlag, Volltext: https://doi.org/https://doi.org/10.5194/acp-19-11687-2019
Verlag: https://www.atmos-chem-phys.net/19/11687/2019/
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Verfasserangaben:Wei Huang, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Thomas Leisner, and Claudia Mohr

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520 |a <p><strong>Abstract.</strong> The 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 (<span class="inline-formula">5.1±3.2</span>&thinsp;<span class="inline-formula">µ</span>g&thinsp;m<span class="inline-formula"><sup>−3</sup></span>) than in the winter period (<span class="inline-formula">8.4±5.6</span>&thinsp;<span class="inline-formula">µ</span>g&thinsp;m<span class="inline-formula"><sup>−3</sup></span>), we find relatively larger mass contributions of organics measured by AMS in summer (<span class="inline-formula">68.8±13.4</span>&thinsp;%) compared to winter (<span class="inline-formula">34.8±9.5</span>&thinsp;%). CIMS mass spectra show OOA compounds in summer have O&thinsp;:&thinsp;C of <span class="inline-formula">0.82±0.02</span> and are more influenced by biogenic emissions, while OOA compounds in winter have O&thinsp;:&thinsp;C of <span class="inline-formula">0.89±0.06</span> and are more influenced by biomass burning emissions. Volatility parametrization analysis shows that OOA in winter is less volatile with higher contributions of low-volatility organic compounds (LVOCs) and extremely low-volatility organic compounds (ELVOCs). We partially explain this by the higher contributions of compounds with shorter carbon chain lengths and a higher number of oxygen atoms, i.e., higher O&thinsp;:&thinsp;C 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&thinsp;:&thinsp;C in winter but may also be related to higher particle viscosity due to the higher contributions of larger-molecular-weight LVOCs and ELVOCs, 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 (SVOCs) 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 the molecular composition and volatility of ambient OA particles and into their potential sources.</p> 
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