Limitations of ozone data assimilation with adjustment of NOx emissions: mixed effects on NO2 forecasts over Beijing and surrounding areas

This study investigates a cross-variable ozone data assimilation (DA) method based on an ensemble Kalman filter (EnKF) that has been used in the companion study to improve ozone forecasts over Beijing and surrounding areas. The main purpose is to delve into the impacts of the cross-variable adjustment of nitrogen oxide (NOx) emissions on the nitrogen dioxide (NO2) forecasts over this region during the 2008 Beijing Olympic Games. A mixed effect on the NO2 forecasts was observed through application of the cross-variable assimilation approach in the real-data assimilation (RDA) experiments. The method improved the NO2 forecasts over almost half of the urban sites with reductions of the root mean square errors (RMSEs) by 15-36aEuro-% in contrast to big increases of the RMSEs over other urban stations by 56-239aEuro-%. Over the urban stations with negative DA impacts, improvement of the NO2 forecasts (with 7aEuro-% reduction of the RMSEs) was noticed at night and in the morning versus significant deterioration during daytime (with 190aEuro-% increase of the RMSEs), suggesting that the negative data assimilation impacts mainly occurred during daytime. Ideal-data assimilation (IDA) experiments with a box model and the same cross-variable assimilation method confirmed the mixed effects found in the RDA experiments. In the same way, NOx emission estimation was improved at night and in the morning even under large biases in the prior emission, while it deteriorated during daytime (except for the case of minor errors in the prior emission). The mixed effects observed in the cross-variable data assimilation, i.e., positive data assimilation impacts on NO2 forecasts over some urban sites, negative data assimilation impacts over the other urban sites, and weak data assimilation impacts over suburban sites, highlighted the limitations of the EnKF under strong nonlinear relationships between chemical variables. Under strong nonlinearity between daytime ozone concentrations and NOx emissions uncertainties (with large biases in the a priori emission), the EnKF may come up with inefficient or wrong adjustments to NOx emissions. The present findings reveal that bias correction is essential for the application of the EnKF in dealing with the data assimilation problem over strong nonlinear system.