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Mountainous regions are often considered pristine environments; however they can be affected by pollutants emitted in more populated and industrialised areas, transported by regional winds. Based on experimental evidence, further supported by modelling tools, here we demonstrate and quantify the impact of air masses transported from the Po Valley, a European atmospheric pollution hotspot, to the northwestern Alps. This is achieved through a detailed investigation of the phenomenology of near-range (a few hundred kilometres), trans-regional transport, exploiting synergies of multi-sensor observations mainly focussed on particulate matter. The explored dataset includes vertically resolved data from atmospheric profiling techniques (automated lidar ceilometers, ALCs), vertically integrated aerosol properties from ground (sun photometer) and space, and in situ measurements (PM10 and PM2.5, relevant chemical analyses, and aerosol size distribution). During the frequent advection episodes from the Po basin, all the physical quantities observed by the instrumental setup are found to significantly increase: the scattering ratio from ALC reaches values >30, aerosol optical depth (AOD) triples, surface PM10 reaches concentrations >100 µg m−3 even in rural areas, and contributions to PM10 by secondary inorganic compounds such as nitrate, ammonium, and sulfate increase up to 28 %, 8 %, and 17 %, respectively. Results also indicate that the aerosol advected from the Po Valley is hygroscopic, smaller in size, and less light-absorbing compared to the aerosol type locally emitted in the northwestern Italian Alps. In this work, the phenomenon is exemplified through detailed analysis and discussion of three case studies, selected for their clarity and relevance within the wider dataset, the latter being fully exploited in a companion paper quantifying the impact of this phenomenology over the long-term (Diémoz et al., 2019). For the three case studies investigated, a high-resolution numerical weather prediction model (COSMO) and a Lagrangian tool (LAGRANTO) are employed to understand the meteorological mechanisms favouring transport and to demonstrate the Po Valley origin of the air masses. In addition, a chemical transport model (FARM) is used to further support the observations and to partition the contributions of local and non-local sources. Results show that the simulations are important to the understanding of the phenomenon under investigation. However, in quantitative terms, modelled PM10 concentrations are 4–5 times lower than the ones retrieved from the ALC and maxima are anticipated in time by 6–7 h. Underestimated concentrations are likely mainly due to deficiencies in the emission inventory and to water uptake of the advected particles not fully reproduced by FARM, while timing mismatches are likely an effect of suboptimal simulation of up-valley and down-valley winds by COSMO. The advected aerosol is shown to remarkably degrade the air quality of the Alpine region, with potential negative effects on human health, climate, and ecosystems, as well as on the touristic development of the investigated area. The findings of the present study could also help design mitigation strategies at the trans-regional scale in the Po basin and suggest an observation-based approach to evaluate the outcome of their implementation.

Chemical and dynamical processes lead to the formation of aerosol layers in the upper planetary boundary layer (PBL) and above it. Through vertical mixing and entrainment into the PBL these layers may contribute to the ground-level particulate matter (PM); however, to date a quantitative assessment of such a contribution has not been carried out. This study investigates this aspect by combining chemical and physical aerosol measurements with WRF/Chem (Weather Research and Forecasting with Chemistry) model simulations. The observations were collected in the Milan urban area (northern Italy) during the summer of 2007. The period coincided with the passage of a meteorological perturbation that cleansed the lower atmosphere, followed by a high-pressure period favouring pollutant accumulation. Lidar observations revealed the formation of elevated aerosol layers and evidence of their entrainment into the PBL. We analysed the budget of ground-level PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 μm) with the help of the online meteorology–chemistry WRF/Chem model, focusing in particular on the contribution of upper-level processes. Our findings show that an important player in determining the upper-PBL aerosol layer is particulate nitrate, which may reach higher values in the upper PBL (up to 30% of the aerosol mass) than in the lower PBL. The nitrate formation process is predicted to be largely driven by the relative-humidity vertical profile, which may trigger efficient aqueous nitrate formation when exceeding the ammonium nitrate deliquescence point. Secondary PM2.5 produced in the upper half of the PBL may contribute up to 7–8 μg m−3 (or 25%) to ground-level concentrations on an hourly basis. The residual aerosol layer above the PBL is also found to potentially play a large role, which may occasionally contribute up to 10–12 μg m−3 (or 40%) to hourly ground-level PM2.5 concentrations during the morning hours. Although the results presented here refer to one relatively short period in one location, this study highlights the importance of considering the interplay between chemical and dynamical processes occurring within and above the PBL when interpreting ground-level aerosol observations.