Role of Upwind Precipitation in Transboundary Pollution and Secondary Aerosol Formation: A Case Study during the KORUS-AQ Field Campaign

Abstract

Abstract Clouds and precipitation play critical roles in wet removal of aerosols and soluble gases in the atmosphere, and hence their accurate prediction largely influences accurate prediction of air pollutants. In this study, the impacts of clouds and precipitation on wet scavenging and long-range transboundary transport of pollutants are examined during the 2016 Korea–United States Air Quality (KORUS-AQ) field campaign using the Weather Research and Forecasting Model coupled with chemistry. Two simulations—one in which atmospheric moisture is constrained and one in which it is not—are performed and evaluated against surface and airborne observations. The simulation with moisture constraints is found to better reproduce precipitation as well as surface PM2.5, whereas the areal extent and amount of precipitation are overpredicted in the simulation without moisture constraints. As a results of overpredicted clouds and precipitation and consequently overpredicted wet scavenging, PM2.5 concentration is generally underpredicted across the model domain in the simulation without moisture constraints. The effects are significant not only in the precipitating region (upwind region, southern China in this study) but also in the downwind region (South Korea) where no precipitation is observed. The difference in upwind precipitation by 77% on average between the two simulations leads to the difference in PM2.5 by ∼39% both in the upwind and downwind regions. The transboundary transport of aerosol precursors, especially nitric acid, has a considerable impact on ammonium-nitrate aerosol formation in the ammonia-rich downwind region. This study highlights that skillful prediction of atmospheric moisture can have ultimate potential to skillful prediction of aerosols across regions.