The role of vertical grid resolution and turbulent diffusion uncertainty on chemical transport modeling

Chemical transport models (CTM) tend to perform poorly in simulating pollution processes under weak turbulent diffusion conditions. In this study, we address this issue from the perspectives of vertical grid resolution and vertical mixing schemes. Three vertical grid resolution configurations (L4, L12, L40) with the CHIMERE model are evaluated during a winter episode, which includes a heavy pollution episode (PE) in the Paris region. The results emphasize the significance of vertical grid resolution, particularly noticeable during nighttime, and consequently impacts CHIMERE simulations under nocturnal stable conditions. Consistent improvement in CTM modeling is observed with refined vertical resolutions and the first layer height based on a simple linear vertical diffusion scheme defined as the initial Kz diffusion (IKD) scheme. Compared to the other two configurations, the finest configuration (referred to as L4-IKD) demonstrates an average improvement in root mean square error of 23.26 % and 25.09 % on regular days (RD) and 62 % and 129 % during PE, respectively. However, simulations using the 1.5-order turbulence kinetic energy (TKE) based eddy diffusivity closure scheme, named the new eddy diffusion (NED), are more sensitive to the first layer height setup. Excessively fine first-layer heights can lead to inaccurate TKE calculations. Generally, models with low vertical grid resolution can reasonably predict air quality on RD or during light pollution events but struggle with heavy PEs. One straightforward enhancement strategy involves adding an extra fine first layer height in CTM simulations, resulting in an average 50.10 % improvement from L4-IKD to L12-IKD during PE. Another strategy is enhancing the model's vertical diffusion scheme, which improved the CTM modeling by 26.67 % compared with IKD during PE under identical vertical grid resolution.