Sources and mixing state of summertime background aerosol in the northwestern Mediterranean basin
Jovanna Arndt1, Jean Sciare2,3, Marc Mallet4, Greg C. Roberts4,5, Nicolas Marchand6, Karine Sartelet7, Karine Sellegri8, François Dulac2, Robert M. Healy9, and John C. Wenger11Department of Chemistry and Environmental Research Institute, University College Cork, Cork, Ireland 2LSCE, Laboratoire des Sciences du Climat et de l’Environnement, Unité Mixte CEA-CNRS-UVSQ, Univ. ParisSaclay, CEA Saclay/Orme des Merisiers 701, F-91191 Gif-sur-Yvette, France 3Energy, Environment and Water Research Center, The Cyprus Institute, 2121 Nicosia, Cyprus 4CNRM, Centre National de Recherches Météorologiques UMR 3589, Météo-France/CNRS, Toulouse, France 5Scripps Institution of Oceanography, Center for Atmospheric Sciences and Physical Oceanography, La Jolla, United States 6Aix Marseille Univ, CNRS, LCE, Marseille, France 7CEREA, Centre d’Enseignement et de Recherche en Environnement Atmosphérique, Joint Laboratory ENPC ParisTech/EDF R&D, Université Paris-Est, Marne la Vallée, France 8LaMP, Laboratoire de Météorologie Physique CNRS UMR6016, Observatoire de Physique du Globe de Clermont-Ferrand, Université Blaise Pascal, Aubière, France 9Environmental Monitoring and Reporting Branch, Ontario Ministry of the Environment and Climate Change, Toronto, Canada
Received: 23 Nov 2016 – Accepted for review: 13 Jan 2017 – Discussion started: 08 Feb 2017
Abstract. An aerosol time-of-flight mass spectrometer (ATOFMS) was employed to provide real-time single particle mixing state and thereby source information for aerosols impacting the western Mediterranean basin during the ChArMEx-ADRIMED and SAF-MED campaigns in summer 2013. The ATOFMS measurements were made at a ground-based remote site on the northern tip of Corsica Island. 27 distinct ATOFMS particle classes were identified and subsequently grouped into 8 general categories: EC-rich (elemental carbon), K-rich, Na-rich, Amines, OC-rich (organic carbon), V-rich, Fe-rich and Ca-rich. Mass concentrations were reconstructed for the ATOFMS particle classes and found to be in good agreement with other co-located quantitative measurements (PM1, black carbon (BC), organic carbon, sulfate mass and ammonium mass). Total ATOFMS reconstructed mass (PM2.5) accounted for 70–90 % of measured PM10 mass and was comprised of regionally transported fossil fuel (EC-rich) and biomass burning (K-rich) particles. The accumulation of these transported particles was favoured by repeated and extended periods of air mass stagnation over the western Mediterranean during the sampling campaigns. The single particle mass spectra proved to be valuable source markers, allowing the identification of fossil fuel and biomass burning combustion sources, and therefore highly complementary to quantitative measurements made by particle-into-liquid sampler ion chromatography (PILS-IC) and an aerosol chemical speciation monitor (ACSM), which have demonstrated that PM1 and PM10 were comprised predominantly of sulfate, ammonium and OC. Good temporal agreement was observed between ATOFMS EC-rich and K-rich particle mass concentrations and combined mass concentrations of BC, sulfate, ammonium and low volatility oxygenated organic aerosol (LV-OOA). This combined information suggests that combustion of fossil fuels and biomass produced primary EC- and OC-containing particles, which then accumulated ammonium, sulfate and alkylamines during regional transport. Three other sources were also identified: local biomass burning, marine and shipping. Local combustion particles (emitted in Corsica) contributed little to PM2.5 particle number and mass concentrations but were easily distinguished from regional combustion particles. Marine emissions comprised fresh and aged sea salt; the former detected mostly during one 5-day event during which it accounted for 50–80 % of sea salt aerosol mass, while the latter detected throughout the sampling period. Dust was not efficiently detected by the ATOFMS, and support measurements showed that it was mainly in the PM2.5–10 fraction. Shipping particles, identified using markers for heavy fuel oil combustion, were associated with regional emissions, and represented only a small fraction of PM2.5 particle number and mass concentration at the site.
Arndt, J., Sciare, J., Mallet, M., Roberts, G. C., Marchand, N., Sartelet, K., Sellegri, K., Dulac, F., Healy, R. M., and Wenger, J. C.: Sources and mixing state of summertime background aerosol in the northwestern Mediterranean basin, Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-1044, in review, 2017.