Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

Abstract:

In this study, we investigate the spatial distribution of PM₁ in the greater London area during the Clean Air for London (ClearfLo) project in winter 2012 by applying two High-Resolution Time-of-Flight Aerosol Mass Spectrometers (HR-ToF-AMS) at a rural site (Detling, Kent) and an urban site (North Kensington, London). While the concentration of organic aerosol (OA) is comparable between the rural and urban sites, the OA sources are distinctly different. Due to elevated domestic heating in the urban area, the concentration of solid fuel OA at the urban site is about twice as high as at the rural site. In contrast, the OOA concentration at the rural site is almost twice that of the urban site. This is likely caused by a steep concentration gradient of OOA when air masses are advected from polluted mainland Europe. Taking advantage of low biogenic emissions in winter, the sources of OOA, which are highly uncertain, are investigated. Combing Positive Matrix Factorization (PMF) analysis and radiocarbon analysis, the majority of OOA is estimated to arise from aged biomass burning. We deploy a suite of instruments to investigate the organic volatility at the rural Detling site. After heating at 250°C in a thermal-denuder (TD), the mass fraction remaining of organics is 16%, which indicates the presence of non-volatile organics. By comparing the OA associated with refractory black carbon (measured by a soot-particle aerosol mass spectrometer) and total OA (measured by a HR-ToF-AMS), we proposed that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon in the atmosphere. Finally, we will discuss the relationship between the volatility and the degree of oxidation of organics.