The impact of evolving synoptic weather patterns on multi-scale transport and sources of persistent high-concentration ozone pollution event in the Yangtze River Delta, China.

High-concentration ozone pollution pose threats to ecosystems and human health. However, there is limited research on the impact of the alternating evolution of synoptic weather patterns (SWPs) on the multi-scale transport processes and sources of ozone. From June 14 to 18, 2018, a rare consecutive ozone pollution plagued in Hefei and broader Yangtze River Delta region (YRD). This study investigates the meteorological factors and sources using in-situ observational data and WRF-Chem model simulations. Analysis reveals a northeastern low-pressure system moving from north to south generated a cold front. This moving cold front facilitated the vertical transport of warm air masses carrying high-concentration ozone originating from North China. Subsequently, Ozone-rich air masses (ORMs) were transported over the YRD, influenced by the eastward movement of the Mongolian high-pressure system. Based on WRF-Chem model with NOx tagging mechanisms and WRF-FLEXPART backward simulations, it is confirmed that a notable atmospheric transport originated from North China region (NCR) to Hefei, especially on June 15. As the Mongolian high-pressure weakens and shifts east-southward, it carried ORMs generated by NOx emissions from the YRD, accumulating over the sea within the range of 120°E to 126°E and 25°N to 30°N. Both WRF-chem model results and TRopospheric Ozone and Precursors from Earth System Sounding (TROPESS) Chemistry Reanalysis dataset Version 2 (TCR-2) revealed the existence of ORMs in this geographic range. Subsequently, the ORMs carried out to sea by the weakened high-pressure system were reintroduced inland, influenced by southeast winds brought about by the peripheral circulation of typhoon "Gaemi". In summary, the alternating evolution of SWPs significantly influences multi-scale ozone transport from both the NCR and the YRD regions, making substantial contributions to this prolonged episode. These findings offer valuable insights for improving regional ozone pollution prevention and control mechanisms.

McPrA - A new gas profile inversion algorithm for MAX-DOAS and apply to 50 m vertical resolution.

Air pollutants represent an environmental and health risk, and the methods for their effective assessment are of the greatest importance. The MAX-DOAS method is a reliable retrieval algorithm, enabling a vertical gas profile analysis. However, the current MAX-DOAS retrieval algorithm heavily relies on the a priori profile, limiting its accuracy. To address this issue, we introduced a novel MAX-DOAS trace gas profile inversion algorithm called McPrA, which is less dependent on the a priori profile. It employs the Monte Carlo method to resolve the problem of optimal estimation of trace gases. The gas vertical column density is obtained from the air mass factor calculated by SCIATRAN. Afterward, the trace gas vertical distribution is retrieved by combining the weight function with the a priori profile. A normalization process is also included to improve the matching of the weight function and the a priori profile. The McPrA algorithm enables greater flexibility in grid modification to achieve a higher vertical resolution of up to 50 m, while sensitivity experiments contribute to determining the optimal configuration of retrieval parameters, with a degree of freedom of over 3.0. Comparative verification experiments indicate that the McPrA algorithm accurately retrieves gas profiles, with a correlation coefficient of over 0.89 for NO2 in the first layer compared to in situ data. Furthermore, comparisons with WRF-Chem and the simulation of synthetic data demonstrate the effectiveness of the McPrA algorithm in accurately retrieving gas profiles.

Study of SO2 measurement based on a dual optical path Fabry-Perot correlation spectroscopy.

This paper investigates a method for measuring SO2 concentration using Fabry-Perot interferometer correlation spectroscopy. In this method, the experimental system is designed as a separated beam, with the beam entering the F-P cavity at two incidence angles simultaneously to match the peak and valley positions of the SO2 absorption cross-section. The system achieves a 2σ detection limit of 28.2 ppm·m(15 cm) at a sampling frequency of 10 Hz. An outfield comparison experiment with the differential optical absorption spectroscopy method shows good agreement for the simultaneous measurement of SO2 concentration from sulfur combustion, with a correlation coefficient of R2 = 0.93. This study introduces a non-dispersive, highly accurate, and fast gas detection technique.

The vertical distribution and potential sources of aerosols in the Yangtze River Delta region of China during open straw burning.

To explore the impact of open straw burning on air quality in the Yangtze River Delta (YRD) and surrounding areas, three key cities in the YRD, namely Hefei, Nanjing, and Shanghai, were selected to observe changes in aerosol characteristics. Based on Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations from May to June 2021, the spatial-temporal distribution and potential sources of aerosol were studied. During the observation period, aerosol optical depth (AOD) in Shanghai was 55.15 % and 29.50 % higher than that in Hefei and Nanjing, respectively. For Shanghai, aerosols accumulated at night, and the aerosol extinction could reach 1.3 km-1 in the morning. The aerosol variations in Hefei and Nanjing were consistent due to the relative conformity of the surrounding environmental conditions (R = 0.84). The vertical distribution of aerosol in all three cities had the same Gaussian shape. The aerosol lifted layers in Nanjing and Shanghai were higher than that in Hefei, with heights of 0.2-0.8 km and 0.2-0.6 km, respectively. The averaged aerosol extinctions for these two cities were 0.34 km-1 and 0.49 km-1, respectively. Pollution source analysis was conducted based on wind field trajectory, satellite observation, and model simulation, taking Hefei as the recipient. The results showed that western Shandong Province, northern Anhui Province, northern Jiangxi Province, central Jiangsu Province, and the central YRD were the most important aerosols sources for Hefei. The contributions of central and southern Jiangsu Province were significantly higher than those of other potential sources, with a WCWTAOD (Meteoinfo concentration weight trajectory) between 1.2 and 3.0. The influence of fine particles produced by open biomass burning inside the YRD was significantly higher than that outside the region (outside contribution: 36.6 %). Regarding the influence between YRD cities, more aerosols were transported from Shanghai to Hefei and Nanjing, with similar transport contributions between Nanjing and Hefei.

Vertical characteristics of NO2 and HCHO, and the ozone formation regimes in Hefei, China.

The research on the mechanism of combined air pollution in the Yangtze-Huaihe region, which is characterized by unique meteorological and geographical conditions and pollution emission characteristics, is still insufficient. We performed an experiment on key pollutants and an ozone formation study in Hefei, which is a pivotal city in the Yangtze-Huaihe region, from September 1 to 20, 2020. The aerosols retrieved via two-dimensional Multi-axis Differential Optical Absorption Spectroscopy (2D-MAX-DOAS) with a Boltzmann-shaped a priori profile had the best agreement with the results of Light Detection and Ranging (LIDAR) and sun-photometer measurements among the three typical a priori profiles (Gaussian, Boltzmann, and exponential shapes). The correlation coefficients of the near-surface gas concentrations retrieved using both 2D-MAX-DOAS and in situ measurements were 0.86 (NO2) and 0.61 (HCHO). The high NO2 and HCHO concentrations were observed at azimuths of 180° and 315° at heights of 0.8-1.5 km, and they may have been emitted by aircrafts. Importantly, the ratio of HCHO to NO2 during a typical pollution episode revealed that the factors controlling the O3 formation changed with altitude: VOCs (surface) to NOx (0.4 km) to transition (1.0 km) to VOCs (1.6 km). Moreover, the effect of VOCs on the O3 generation was stronger than that of NOx, especially in the downtown area of Hefei. When the ratio of HCHO to NO2 was 3.55-7.46, the ozone concentration in Hefei could be controlled well, especially at the optimal value of 5.50.