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Volume 15, issue 19 | Copyright

Special issue: The Pan European Gas-Aerosols Climate Interaction Study...

Atmos. Chem. Phys., 15, 11327-11340, 2015
https://doi.org/10.5194/acp-15-11327-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 12 Oct 2015

Research article | 12 Oct 2015

Organic aerosol evolution and transport observed at Mt. Cimone (2165 m a.s.l.), Italy, during the PEGASOS campaign

M. Rinaldi1, S. Gilardoni1, M. Paglione1, S. Sandrini1, S. Fuzzi1, P. Massoli2, P. Bonasoni1, P. Cristofanelli1, A. Marinoni1, V. Poluzzi3, and S. Decesari1 M. Rinaldi et al.
  • 1National Research Council, Institute of Atmospheric Sciences and Climate, Bologna, Italy
  • 2Aerodyne Research Inc., Billerica, MA, USA
  • 3Centro Tematico Regionale Aree Urbane, Arpa Emilia-Romagna, Bologna, Italy

Abstract. High-resolution aerosol mass spectrometer measurements were performed, for the first time, at the Mt. Cimone Global Atmosphere Watch (GAW) station between June and July 2012, within the EU project PEGASOS and the ARPA–Emilia-Romagna project SUPERSITO. Submicron aerosol was dominated by organics (63 %), with sulfate, ammonium and nitrate contributing the remaining 20, 9 and 7 %, respectively. Organic aerosol (OA) was in general highly oxygenated, consistent with the remote character of the site; our observations suggest that oxidation and secondary organic aerosol (SOA) formation processes occurred during aerosol transport to high altitudes. All of the aerosol component concentrations as well as the OA elemental ratios showed a clear daily trend, driven by the evolution of the planetary boundary layer (PBL) and by the mountain wind regime. Higher loadings and lower OA oxidation levels were observed during the day, when the site was within the PBL, and therefore affected by relatively fresh aerosol transported from lower altitudes. Conversely, lower loadings and higher OA oxidation levels were observed at night, when the top of Mt. Cimone resided in the free troposphere although affected by the transport of residual layers on several days of the campaign. Analysis of the elemental ratios in a Van Krevelen space shows that OA oxidation follows a slope comprised between −0.5 and −1, consistent with addition of carboxylic groups, with or without fragmentation of the parent molecules. The increase of carboxylic groups during OA ageing is confirmed by the increased contribution of organic fragments containing more than one oxygen atom in the free troposphere night-time mass spectra. Finally, positive matrix factorization was able to deconvolve the contributions of relatively fresh OA (OOAa) originating from the PBL, more aged OA (OOAb) present at high altitudes during periods of atmospheric stagnation, and very aged aerosols (OOAc) transported over long distances in the free troposphere.

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This work highlights the important contribution of organic aerosols to the composition of submicron particles at remote mountain sites. Moreover, it confirms the importance of regional-scale physical and chemical processes and of transboundary transport in determining the background aerosol composition at rural European sites.
This work highlights the important contribution of organic aerosols to the composition of...
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