Sensitivity of spatial aerosol particle distributions to the boundary conditions in the PALM model system 6.0

High-resolution modelling is needed to understand urban air quality and pollutant dispersion in detail. Recently, the PALM model system 6.0, which is based on large-eddy simulation (LES), was extended with the detailed Sectional Aerosol module for Large Scale Applications (SALSA) v2.0 to enable studying the complex interactions between the turbulent flow field and aerosol dynamic processes. This study represents an extensive evaluation of the modelling system against the horizontal and vertical distributions of aerosol particles measured using a mobile laboratory and a drone in an urban neighbourhood in Helsinki, Finland. Specific emphasis is on the model sensitivity of aerosol particle concentrations, size distributions and chemical compositions to boundary conditions of meteorological variables and aerosol background concentrations. The meteorological boundary conditions are taken from both a numerical weather prediction model and observations, which occasionally differ strongly. Yet, the model shows good agreement with measurements (fractional bias < 0.67, normalised mean squared error < 6, fraction of the data within a factor of 2 > 0.3, normalised mean bias factor < 0.25 and normalised mean absolute error factor < 0.35) with respect to both horizontal and vertical distribution of aerosol particles, their size distribution and chemical composition. The horizontal distribution is most sensitive to the wind speed and atmospheric stratification, and vertical distribution to the wind direction. The aerosol number size distribution is mainly governed by the flow field along the main street with high traffic rates and in its surroundings by the background concentrations. The results emphasise the importance of correct meteorological and aerosol background boundary conditions, in addition to accurate emission estimates and detailed model physics, in quantitative high-resolution air pollution modelling and future urban LES studies.