Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe

نویسندگان

  • Elham Baranizadeh
  • Benjamin N. Murphy
  • Jan Julin
  • Saeed Falahat
  • Carly L. Reddington
  • Antti Arola
  • Lars Ahlm
  • Santtu Mikkonen
  • Christos Fountoukis
  • David Patoulias
  • Andreas Minikin
  • Thomas Hamburger
  • Ari Laaksonen
  • Spyros N. Pandis
  • Hanna Vehkamäki
  • Kari E. J. Lehtinen
  • Ilona Riipinen
چکیده

The particle formation scheme within PMCAMxUF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4– NH3–H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions–Long-Range Experiment)campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiativetransfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation Published by Copernicus Publications on behalf of the European Geosciences Union. 2742 E. Baranizadeh et al.: Implementation of state-of-the-art ternary new-particle formation scheme above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.

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تاریخ انتشار 2016