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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 18, issue 3 | Copyright
Atmos. Chem. Phys., 18, 2155-2174, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 14 Feb 2018

Research article | 14 Feb 2018

Insights into organic-aerosol sources via a novel laser-desorption/ionization mass spectrometry technique applied to one year of PM10 samples from nine sites in central Europe

Kaspar R. Daellenbach1, Imad El-Haddad1, Lassi Karvonen1, Athanasia Vlachou1, Joel C. Corbin1, Jay G. Slowik1, Maarten F. Heringa1, Emily A. Bruns1, Samuel M. Luedin2,a, Jean-Luc Jaffrezo3, Sönke Szidat4, Andrea Piazzalunga5,b, Raquel Gonzalez6, Paola Fermo6, Valentin Pflueger2, Guido Vogel2, Urs Baltensperger1, and André S. H. Prévôt1 Kaspar R. Daellenbach et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
  • 2MABRITEC AG, Riehen, Switzerland
  • 3Université Grenoble Alpes, CNRS, IGE, 38000 Grenoble, France
  • 4Department of Chemistry and Biochemistry & Oeschger Centre for Climate Change Research, University of Bern, 3012 Bern, Switzerland
  • 5Università degli Studi di Milano-Bicocca, 20126 Milan, Italy
  • 6Università degli Studi di Milano, 20133 Milan, Italy
  • anow at: University of Geneva, 1211 Geneva, Switzerland
  • bnow at: Water and Soil Lab, 24060 Entratico, Italy

Abstract. We assess the benefits of offline laser-desorption/ionization mass spectrometry in understanding ambient particulate matter (PM) sources. The technique was optimized for measuring PM collected on quartz-fiber filters using silver nitrate as an internal standard for mz calibration. This is the first application of this technique to samples collected at nine sites in central Europe throughout the entire year of 2013 (819 samples). Different PM sources were identified by positive matrix factorization (PMF) including also concomitant measurements (such as NOx, levoglucosan, and temperature). By comparison to reference mass spectral signatures from laboratory wood burning experiments as well as samples from a traffic tunnel, three biomass burning factors and two traffic factors were identified. The wood burning factors could be linked to the burning conditions; the factors related to inefficient burns had a larger impact on air quality in southern Alpine valleys than in northern Switzerland. The traffic factors were identified as primary tailpipe exhaust and most possibly aged/secondary traffic emissions. The latter attribution was supported by radiocarbon analyses of both the organic and elemental carbon. Besides these sources, factors related to secondary organic aerosol were also separated. The contribution of the wood burning emissions based on LDI-PMF (laser-desorption/ionization PMF) correlates well with that based on AMS-PMF (aerosol mass spectrometer PMF) analyses, while the comparison between the two techniques for other components is more complex.

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A novel offline LDI-MS method was developed to analyse particulate matter (PM) collected at multiple sites in central Europe during the entire year of 2013. PM sources were identified by positive matrix factorization. Wood burning emissions were separated according to the burning conditions; inefficient burns had a larger impact on air quality in southern Alpine valleys than in northern Switzerland. Moreover, primary tailpipe exhaust was distinguished from aged/secondary traffic emissions.
A novel offline LDI-MS method was developed to analyse particulate matter (PM) collected at...