Implementation of an On-Line Reactive Source Apportionment (ORSA) Algorithm in the FARM Chemical-Transport Model and Application over Multiple Domains in Italy

Abstract

A source apportionment scheme based on gas and aerosol phase reactive tracers has been implemented in the chemical-transport model FARM, to efficiently estimate contributions of different sources to ambient concentrations. The on-line scheme deals with all the main processes that the chemical species undergo in the model, to enhance consistency with the calculation of bulk concentrations. The fate of precursors through gas-phase chemical reactions is followed by an efficient solver that determines their incremental reactivity, while the contributions to the secondary particulate species from their gaseous precursors is determined by assuming the thermodynamic equilibrium between the two phases. The paper details the new employed methodologies and illustrates the application of the apportionment scheme (based on 6 source sectors) to PM10 and O3, simulated on three domains of different dimensions in Italy, all sharing the same horizontal resolution and a common region (Lombardy). Spatial patterns of results show, on average, a relevant contribution of heating on PM10 concentration in January, with local hotspots dominated by road traffic. Contributions appear consistent in the three simulated domains, apart from the boundary conditions, influenced by the dimension of the domain. Hourly series of contributions to O3 concentrations in July at three selected sites show the dominance of boundary conditions, underlining the large scale of O3 formation. Finally, for PM10 components, the resulting sectorial contributions are compared with the impacts computed via the brute force method, showing that results are similar for elemental carbon and sulfate, while they are different for nitrate and ammonium, due to a different allocation of contributions and impacts between the methods. Each approach responds in principle to a different purpose, and their combined use provides possibly a wide set of information useful for addressing the different air quality management needs.