Multi-method determination of the below-cloud wet scavenging coefficients of aerosols in Beijing, China

Abstract

Wet scavenging is one of the most efficient processes for removing aerosols from the atmosphere. This process is not well constrained in chemical transport models (CTMs) due to a paucity of localized parameterization regarding the below-cloud wet scavenging coefficient (BWSC). Here we conducted field measurements of the BWSC during the Atmospheric Pollution and Human Health Beijing (APHH-Beijing) campaign of 2016. Notably, the observed BWSC values based on the updated aerosol mass balance agree well with another estimation technique, and they fall in a range of 10-5 s-1. The measurement in this winter campaign, combined with that in summer of 2014, supported an exponential power distribution of BWSCs with rainfall intensity. The observed parameters were also compared with both the theoretical calculations and modeling results. We found that the theoretical estimations can effectively characterize the observed BWSCs of aerosols with sizes smaller than 0.2 μ m and larger than 2.5 μ m. However, the theoretical estimations were an order of magnitude lower than observed BWSCs within 0.2-2.5 μ m, a domain size range of urban aerosols. Such an underestimation of BWSC through a theoretical method has been confirmed not only in APHHBeijing campaign but also in all the rainfall events in summer of 2014. Since the model calculations usually originated from the theoretical estimations with simplified scheme, the significantly lower BWSC could well explain the underprediction of wet depositions in polluted regions as reported by the Model Inter-Comparison Study for Asia (MICS-Asia) and the global assessment of the Task Force on Hemispheric Transport of Atmospheric Pollutants (TF-HTAP). The findings highlighted that the wet deposition module in the CTMs requires improvement based on field measurement estimation to construct a more reasonable simulation scheme for BWSC, especially in polluted regions.