WRF-CHEM Model Sensitivity To Chemical Mechanisms Choice In Reconstructing Aerosol Optical Properties

Abstract

In the framework of the AQMEII initiative WRF-Chem has been applied over Europe adopting two chemical configurations for the calendar year 2010. The first one employed the RADM2 gas-phase chemistry and MADE/SORGAM aerosol module, while the second one implemented the CBM-Z gaseous parameterization and MOSAIC aerosol chemistry. Configurations shared the same domain, meteorological setups and input data. The Comparison demonstrated that CBM-Z has a more efficient ozone-NO titration than RADM2 in regions with sufficiently high levels of NOx and VOCs. At the same time, CBM-Z is found to have a more effective NO2 + OH reaction. The parameterization of the relative humidity of deliquescence point has a strong impact on HNO3 and NO3 concentrations over Europe, particularly over the sea. The MADE approach showed to be more efficient than MOSAIC. Differently, particulate sulfate and SO2 ground concentrations proved to be more influenced by the heterogeneous SO2 cloud oxidation. PM10 and PM2.5 have shown similar results for MOSAIC and MADE/SORGAM, even though some differences were found in the dust and sea salt size partitioning between modes and bins. Indeed, in MADE the sea salt was distributed only in the coarse fraction, while the dust emissions were distributed mainly in the fine fraction. Finally, different chemical mechanisms give different Aerosol Optical Depths (AOD). WRF-Chem is found to under predict the AODs in both configurations because of the misrepresentation of the dust coarse particle, as shown by the analysis of the relationship between the Angström exponent and the AOD bias. Differently, when the AOD is dominated by fine particles, the differences in model performance are more evident, with MADE/SORGAM generally performing better than MOSAIC. Indeed the higher availability of both sulfate and nitrate has a significant influence on reconstruction of the AOD estimations. This paper shows the great importance of chemical mechanisms in both gaseous and aerosols predictions, as well as in the calculation of aerosol optical properties.