Articles | Volume 15, issue 5
Atmos. Chem. Phys., 15, 2629–2649, 2015
Atmos. Chem. Phys., 15, 2629–2649, 2015

Research article 09 Mar 2015

Research article | 09 Mar 2015

How much is particulate matter near the ground influenced by upper-level processes within and above the PBL? A summertime case study in Milan (Italy) evidences the distinctive role of nitrate

G. Curci1, L. Ferrero2, P. Tuccella1, F. Barnaba3, F. Angelini4, E. Bolzacchini2, C. Carbone5, H. A. C. Denier van der Gon6, M. C. Facchini5, G. P. Gobbi3, J. P. P. Kuenen6, T. C. Landi5, C. Perrino7, M. G. Perrone2, G. Sangiorgi2, and P. Stocchi5 G. Curci et al.
  • 1CETEMPS Centre of Excellence, Department of Physical and Chemical Sciences, University of L'Aquila, L'Aquila, Italy
  • 2POLARIS Research Centre, Department of Earth and Environmental Sciences, University of Milano Bicocca, Milano, Italy
  • 3Institute for Atmospheric and Climate Sciences (ISAC), National Research Council (CNR), Rome, Italy
  • 4Italian National Agency for New Technologies, Energy and Sustainable Economic Development (ENEA), Rome, Italy
  • 5Institute for Atmospheric and Climate Sciences (ISAC), National Research Council (CNR), Bologna, Italy
  • 6TNO Climate, Air and Sustainability, Princetonlaan 6, 3584 CB Utrecht, the Netherlands
  • 7Institute of Atmospheric Pollution Research (IIA), National Research Council (CNR), Rome, Italy

Abstract. 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.

Short summary
Particulate matter (PM) at ground level is of primary concern for the quality of the air we breathe. Most direct sources of PM are near the ground, but an important fraction of PM is produced by photochemical processes happening also in the upper atmospheric layers. We investigated the contribution of those layers to the PM near the ground and found a significant impact. Nitrate is a major player in the “vertical direction”, owing to its sensitivity to ambient temperature and relative humidity.
Final-revised paper