Comment on acp-2022-842

Abstract

Atmospheric aerosol particles are a complex combination of primary emitted sources (biogenic and anthropogenic) and secondary aerosol resulting from the aging processes such as condensation, coagulation, and cloud processing. To better understand their sources, investigations have been focused on source identification in urban areas in the past, while rural background stations are normally less impacted by surrounding anthropogenic sources. Therefore, they are predisposed for studying the impact of long-range transport of anthropogenic aerosols. Moreover, long-term measurements can help to study the potential temporal changes in the sources. Here, the chemical composition and organic aerosol sources of submicron aerosol particles were investigated at the Central European rural-background research station, Melpitz, using a one yearlong dataset determined by an aerosol chemical speciation monitor (ACSM) and a multi-angle absorption photometer (MAAP) from September 2016 to August 2017. Melpitz represents due to its location the Central European aerosol. It is an ideal location to investigate the impact of long-range transport, since the location is influenced by less polluted air masses from westerly directions and more polluted continental air masses from Eastern Europe. The organic aerosol (OA) dominated the submicron particle mass concentration and showed strong seasonal variability ranging from 39 % (in winter) to 58 % (in summer). It was followed by sulphate (15 % and 20 %) and nitrate (24 % and 11 %). The OA source identification was performed using rolling positive matrix factorisation (PMF) approach to account for the potential temporal changes in the source profile (SoFi Pro). It was possible to split OA into five-factors with a distinct temporal variability and mass spectral signature. Three were associated to anthropogenic primary OA (POA) sources: hydrocarbon-like OA (HOA, 5.2 % of OA mass in winter and 6.8 % in summer), biomass burning OA (BBOA, 10.6 % and 6.1 %) and coal combustion OA (CCOA, 23 % and 8.7 %). Another two are secondary/processed oxygenated OA (OOA) sources: less-oxidized OOA (LO-OOA, 28.4 % and 36.7 %) and more-oxidized OOA (MO-OOA, 32.8 % and 41.8 %). Since equivalent black carbon (eBC) was clearly associated with the identified POA factors (sum of HOA, BBOA and CCOA, R2= 0. 87), eBC’s contribution to each of the POA factors was achieved using a multi-linear regression model. Consequently, CCOA represented the main anthropogenic sources of carbonaceous aerosol (sum of OA and eBC) not only during winter (56 % of POA in winter) but also in summer (13 % of POA in summer), followed by BBOA (29 % and 69 % of POA in winter and summer, respectively) and HOA (15 % and 18 % of POA in winter and summer, respectively). A seasonal air mass cluster analysis was used to understand the geographical origins of the different aerosol types and show that during both winter and summer time, PM1 (PM with aerodynamic diameter smaller than 1 µm) air masses with eastern influence was always associated with the highest mass concentration and the highest coal combustion fraction. Since during winter time, CCOA is a combination of domestic heating and power plants emissions, the summer contribution of CCOA emphasises the critical importance of coal power plants emissions to rural background aerosols and its impact on air quality, through long-range transportation.