Across land, sea, and mountains: sulphate aerosol sources and transport dynamics over the northern Apennines

Abstract

In this study, we combine aerosol observations with high-resolution Eulerian (WRF-CHIMERE) and Lagrangian (FLEXPART) modelling to investigate the source regions, emission sources, transport pathways, and chemical transformation of sulphate aerosols at the high-altitude Monte Cimone station during July 2017. Our analysis shows that marine air masses are linked to higher levels of sulphate at Monte Cimone. In particular, the sea plays a dominant role in enhancing the oxidation of sulphur dioxide (SO₂) into sulphate due to prolonged exposure to elevated hydroxyl radical (OH) concentrations over the sea. At the same time, sensitivity simulations reveal that industrial emissions contribute significantly to sulphate levels at Monte Cimone, even when air masses have spent a long time travelling over the sea. Furthermore, examination of vertical atmospheric dynamics indicates that free tropospheric air masses favour higher concentrations of sulphuric acid likely due to lower condensation sink (CS) conditions in the free troposphere (FT). In contrast, boundary layer conditions were found to enhance the transport of dimethyl sulphide (DMS) oxidation products, meaning that, over the Mediterranean Sea, DMS and its oxidation products do not reach the FT efficiently. Our results highlight the complex interaction between marine and terrestrial sources, atmospheric chemistry, and transport mechanisms in shaping sulphate aerosol levels at high-altitude sites. They also provide valuable insights into sulphate sources and transport processes over large geographical areas.