PhD in Physics
Thesis defended on 29th June 2018
Département Sciences de l'Atmosphère et Génie de l'Environnement (SAGE)
Chemical characterization, sources and origins of secondary inorganic aerosols measured at an urban site in Northern France
Tropospheric fine particles with aerodynamic diameters less than 2.5 µm (PM2.5) may impact health, climate and ecosystems. Secondary inorganic (SIA) and organic aerosols (OA) contribute largely to PM2.5. To understand their formation and origin, a 1-year campaign (August 2015 to July 2016) of inorganic precursor gases and PM2.5 water-soluble ions was performed at an hourly resolution at a suburban site in northern France using a MARGA 1S, complemented by mass concentrations of PM2.5, Black Carbon, nitrogen oxides and trace elements. The highest levels of ammonium nitrate (AN) and sulfate were observed at night in spring and during daytime in summer, respectively. A source apportionment study performed by positive matrix factorization (PMF) determined 8 source factors, 3 having a regional origin (sulfate-rich, nitrate-rich, marine) contributing to PM2.5 mass for 73-78%; and 5 a local one (road traffic, biomass combustion, metal industry background, local industry and dust) (22-27%). In addition, a HR-ToF-AMS (aerosol mass spectrometer) and a SMPS (particle sizer) were deployed during an intensive winter campaign, to gain further insight on OA composition and new particle formation, respectively. The application of PMF to the AMS OA mass spectra allowed identifying 5 source factors: hydrocarbon-like (15%), cooking-like (11%), oxidized biomass burning (25%), less- and more-oxidized oxygenated factors (16% and 33%, respectively). Combining the SMPS size distribution with the chemical speciation of the aerosols and precursor gases allowed the identification of nocturnal new particle formation (NPF) events associated to the formation of SIA, in particular AN.
Thesis supervisors :
Véronique RIFFAULT (SAGE), Esperanza PERDRIX (SAGE)