Air pollutants seriously impact climate change and human health. In this study, the gridpoint statistical interpolation (GSI) three-dimensional variational data assimilation system was extended from ground data to vertical profile data, which reduced the simulation error of the model in the vertical layer. The coupled GSI-Lidar-WRF-Chem system was used to improve the accuracy of fine particulate matter (PM2.5) simulation during a wintertime heavy pollution event in the North China Plain in late November 2017. In this experiment, two vehicle-mounted Lidar instruments were utilized to make synchronous observations around the 6th Ring Road of Beijing, and five ground-based Lidars were used for long-term network observations on the North China Plain. Data assimilation was then performed using the PM2.5 vertical profile retrieved from the seven Lidars. Compared with the model results, the correlation of assimilation increased from 0.74–0.86, and the root-mean-square error decreased by 36.6%. Meanwhile, the transport flux and transport flux intensity of the PM2.5 were analyzed, which revealed that the PM2.5 around the 6th Ring Road of Beijing was mainly concentrated below 1.8 km, and there were obvious double layers of particles. Particulates in the southwest were mainly input, while those in the northeast were mainly output. Both the input and output heights were around 1 km, although the input intensity was higher than the output intensity. The GSI-Lidar-WRF-Chem system has great potential for air quality simulation and forecasting.

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Abstract. Aerosol vertical stratification is important for global climate and planetary boundary layer (PBL) stability, and no single method can obtain spatiotemporally continuous vertical profiles. This paper develops an online data assimilation (DA) framework for the Eulerian atmospheric chemistry-transport model (CTM) Nested Air Quality Prediction Model System (NAQPMS) with the Parallel Data Assimilation Framework (PDAF) as the NAQPMS-PDAF for the first time. Online coupling occurs based on a memory-based way with two-level parallelization, and the arrangement of state vectors during the filter is specifically designed. Scaling tests demonstrate that the NAQPMS-PDAF can make efficient use of parallel computational resources for up to 25 000 processors with a weak scaling efficiency of up to 0.7. The 1-month long aerosol extinction coefficient profiles measured by the ground-based lidar and the concurrent hourly surface PM2.5 are solely and simultaneously assimilated to investigate the performance and application of the DA system. The hourly analysis and subsequent 1 h simulation are validated through lidar and surface PM2.5 measurements assimilated and not assimilated. The results show that lidar DA can significantly improve the underestimation of aerosol loading, especially at a height of approximately 400 m in the free-running (FR) experiment, with the mean bias (BIAS) changing from −0.20 (−0.14) km−1 to −0.02 (−0.01) km−1 and correlation coefficients increasing from 0.33 (0.28) to 0.91 (0.53) averaged over sites with measurements assimilated (not assimilated). Compared with the FR experiment, simultaneously assimilating PM2.5 and lidar can have a more consistent pattern of aerosol vertical profiles with a combination of surface PM2.5 and lidar, independent extinction coefficients from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), and aerosol optical depth (AOD) from the Aerosol Robotic Network (AERONET). Lidar DA has a larger temporal impact than that in PM2.5 DA but has deficiencies in subsequent quantification on the surface PM2.5. The proposed NAQPMS-PDAF has great potential for further research on the impact of aerosol vertical distribution.

This paper studied the method for converting the aerosol extinction to the mass concentration of particulate matter (PM) and obtained the spatio-temporal distribution and transportation of aerosol, nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) based on multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations in Dalian (38.85°N, 121.36°E), Qingdao (36.35°N, 120.69°E), and Shanghai (31.60°N, 121.80°E) from 2019 to 2020. The PM2.5 measured by the in situ instrument and the PM2.5 simulated by the conversion formula showed a good correlation. The correlation coefficients R were 0.93 (Dalian), 0.90 (Qingdao), and 0.88 (Shanghai). A regular seasonality of the three trace gases is found, but not for aerosols. Considerable amplitudes in the weekly cycles were determined for NO2 and aerosols, but not for SO2 and HCHO. The aerosol profiles were nearly Gaussian, and the shapes of the trace gas profiles were nearly exponential, except for SO2 in Shanghai and HCHO in Qingdao. PM2.5 presented the largest transport flux, followed by NO2 and SO2. The main transport flux was the output flux from inland to sea in spring and winter. The MAX-DOAS and the Copernicus Atmosphere Monitoring Service (CAMS) models’ results were compared. The overestimation of NO2 and SO2 by CAMS is due to its overestimation of near-surface gas volume mixing ratios.

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