Increase of secondary organic aerosol over four years in an urban
environment
Abstract. The evolution of fine aerosol (PM1) species as well as the contribution of potential sources to the total organic aerosol (OA) at an urban background site (Palau Reial, PR, 80 m a.s.l) in the western Mediterranean basin (WMB) was investigated. For this purpose, an aerosol chemical speciation monitor (ACSM) was deployed to acquire real-time measurements for two one-year periods: May 2014–May 2015 (period A) and Sep 2017–Oct 2018 (period B). Total PM1 concentrations showed a slight decrease (from 10.1 to 9.6 µg · m−3 from A to B), although the relative contribution of both inorganic and organic compounds varied significantly. Regarding inorganic compounds, SO42−, black carbon and NH4+ showed a significant decrease from period A to B, whilst NO3− concentration was found higher in B. Source apportionment revealed OA was 46 % and 70 % of secondary origin (SOA) in periods A and B, respectively. Two oxygenated secondary sources (OOA) were differentiated by their oxidation status (i.e. aging): less-oxidized (LO-OOA) and more-oxidized (MO-OOA). Disregarding winter periods, where LO-OOA production is not favoured, LO-OOA transformation into MO-OOA was found more effective in period B. The highest MO-OOA-to-LO-OOA ratio (1.5) was found in September–October 2018, implying an accumulation effect after the high temperature and solar radiation conditions in the summer season. In addition, SOA was found sensitive to a NOx-polluted ambient and to other pollutants, especially to ozone, which could be enhancing its production specially during afternoon hours. The anthropogenic primary OA sources identified, cooking-like OA (COA), hydrocarbon-like OA (HOA), and biomass burning OA (BBOA), decreased from period A to B in both absolute concentrations and relative contribution (as a whole, 44 % and 40 %, respectively). However, their concentrations and proportion to OA grow rapidly during highly-polluted episodes. The influence of certain atmospheric episodes on OA sources was also assessed. Both SOA factors seem linked with long and medium-range circulations, especially those coming from inland Europe and the Mediterranean (triggering mainly MO-OOA) and summer breeze-driven regional circulation (triggering mainly LO-OOA). In contrast, POA pollution is enhanced either during air-cleaning episodes or stagnation anticyclonic events.