Chemical Data Assimilation With Aqueous Chemistry in WRF-Chem Coupled With WRFDA (V4.4.1)

This study introduces a new chemistry option in the Weather Research and Forecasting model data assimilation (WRFDA) system, coupled with the WRF-Chem model (Version 4.4.1), to incorporate aqueous chemistry (AQCHEM) in the assimilation of ground-level chemical measurements. The new DA capability includes the integration of aqueous-phase aerosols from the Regional Atmospheric Chemistry Mechanism (RACM) gas chemistry, the Modal Aerosol Dynamics Model for Europe (MADE) aerosol chemistry, and the Volatility Basis Set (VBS) for secondary organic aerosol production. The RACM-MADE-VBS-AQCHEM scheme facilitates aerosol-cloud-precipitation interactions by activating aerosol particles in cloud water during the model simulation. With the goal of enhancing air quality forecasting in cloudy conditions, this new implementation is demonstrated in the weakly coupled three-dimensional variational data assimilation (3D-Var) system through regional air quality cycling over East Asia. Surface particulate matter (PM) concentrations and four gas species (SO2, NO2, O3, and CO) are assimilated every 6 hr for the month of March 2019. The results show that including aqueous-phase aerosols in both the analysis and forecast can represent aerosol wet removal processes associated with cloud development and rainfall production. During a pollution event with high cloud cover, simulations without aerosols defined in cloud water exhibit significantly higher values for liquid water path, and surface PM10 (PM2.5) concentrations are overestimated by a factor of 10 (3) when wet scavenging processes dominate. On the contrary, AQCHEM proves to be helpful in simulating the wet deposition of aerosols, accurately predicting the evolution of surface PM concentrations without such overestimation. Major air pollution events over the Korean peninsula are often observed in association with significant cloud cover, especially over the Yellow Sea to the west of the peninsula. Cloudy conditions pose challenges for both remote sensing observations and model predictions, but the inclusion of aqueous-phase (or cloud-borne) aerosols in the WRF-Chem/Weather Research and Forecasting model data assimilation system improves the simulation of aerosol wet scavenging, leading to improved predictions of surface particulate matter concentrations that were otherwise substantially overestimated. The Weather Research and Forecasting (WRF)-Chem/WRF model data assimilation 3D-Var system (V4.4.1) is extended for chemical data assimilation with aqueous chemistry using the Regional Atmospheric Chemistry Mechanism-Modal Aerosol Dynamics Model for Europe-Volatility Basis Set scheme Surface PM2.5, PM10, SO2, NO2, O3, and CO concentrations are assimilated in the coupled system The inclusion of aqueous-phase aerosols in air quality cycling enhances the simulation of aerosol wet deposition in cloudy conditions