Full-coverage mapping and spatiotemporal variations of ground-level ozone (O3) pollution from 2013 to 2020 across China

Ozone (O₃) is an important trace and greenhouse gas in the atmosphere, posing a threat to the ecological environment and human health at the ground level. Large-scale and long-term studies of O₃ pollution in China are few due to highly limited direct ground and satellite measurements. This study offers a new perspective to estimate ground-level O₃ from solar radiation intensity and surface temperature by employing an extended ensemble learning of the space-time extremely randomized trees (STET) model, together with ground-based observations, remote sensing products, atmospheric reanalysis, and an emission inventory. A full-coverage (100%), high-resolution (10 km) and high-quality daily maximum 8-h average (MDA8) ground-level O₃ dataset covering China (called ChinaHighO₃) from 2013 to 2020 was generated. Our MDA8 O₃ estimates (predictions) are reliable, with an average out-of-sample (out-of-station) coefficient of determination of 0.87 (0.80) and root-mean-square error of 17.10 (21.10) μg/m³ in China. The unique advantage of the full coverage of our dataset allowed us to accurately capture a short-term severe O₃ pollution exposure event that took place from 23 April to 8 May in 2020. Also, a rapid increase and recovery of O₃ concentrations associated with variations in anthropogenic emissions were seen during and after the COVID-19 lockdown, respectively. Trends in O₃ concentration showed an average growth rate of 2.49 μg/m³/yr (p < 0.001) from 2013 to 2020, along with the continuous expansion of polluted areas exceeding the daily O₃ standard (i.e., MDA8 O₃ = 160 μg/m³). Summertime O₃ concentrations and the probability of occurrence of daily O₃ pollution have significantly increased since 2015, especially in the North China Plain and the main air pollution transmission belt (i.e., the "2 + 26” cities). However, a decline in both was seen in 2020, mainly due to the coordinated control of air pollution and ongoing COVID-19 effects. This carefully vetted and smoothed dataset is valuable for studies on air pollution and environmental health in China.

Separating Daily 1 km PM2.5 Inorganic Chemical Composition in China since 2000 via Deep Learning Integrating Ground, Satellite, and Model Data.

Fine particulate matter (PM2.5) chemical composition has strong and diverse impacts on the planetary environment, climate, and health. These effects are still not well understood due to limited surface observations and uncertainties in chemical model simulations. We developed a four-dimensional spatiotemporal deep forest (4D-STDF) model to estimate daily PM2.5 chemical composition at a spatial resolution of 1 km in China since 2000 by integrating measurements of PM2.5 species from a high-density observation network, satellite PM2.5 retrievals, atmospheric reanalyses, and model simulations. Cross-validation results illustrate the reliability of sulfate (SO42-), nitrate (NO3-), ammonium (NH4+), and chloride (Cl-) estimates, with high coefficients of determination (CV-R2) with ground-based observations of 0.74, 0.75, 0.71, and 0.66, and average root-mean-square errors (RMSE) of 6.0, 6.6, 4.3, and 2.3 µg/m3, respectively. The three components of secondary inorganic aerosols (SIAs) account for 21% (SO42-), 20% (NO3-), and 14% (NH4+) of the total PM2.5 mass in eastern China; we observed significant reductions in the mass of inorganic components by 40-43% between 2013 and 2020, slowing down since 2018. Comparatively, the ratio of SIA to PM2.5 increased by 7% across eastern China except in Beijing and nearby areas, accelerating in recent years. SO42- has been the dominant SIA component in eastern China, although it was surpassed by NO3- in some areas, e.g., Beijing-Tianjin-Hebei region since 2016. SIA, accounting for nearly half (∼46%) of the PM2.5 mass, drove the explosive formation of winter haze episodes in the North China Plain. A sharp decline in SIA concentrations and an increase in SIA-to-PM2.5 ratios during the COVID-19 lockdown were also revealed, reflecting the enhanced atmospheric oxidation capacity and formation of secondary particles.

Ground-level gaseous pollutants (NO2, SO2, and CO) in China: daily seamless mapping and spatiotemporal variations

Gaseous pollutants at the ground level seriously threaten the urban air quality environment and public health. There are few estimates of gaseous pollutants that are spatially and temporally resolved and continuous across China. This study takes advantage of big data and artificial-intelligence technologies to generate seamless daily maps of three major ambient pollutant gases, i.e., NO2, SO2, and CO, across China from 2013 to 2020 at a uniform spatial resolution of 10 km. Cross-validation between our estimates and ground observations illustrated a high data quality on a daily basis for surface NO2, SO2, and CO concentrations, with mean coefficients of determination (root-mean-square errors) of 0.84 (7.99 µg m-3), 0.84 (10.7 µg m-3), and 0.80 (0.29 mg m-3), respectively. We found that the COVID-19 lockdown had sustained impacts on gaseous pollutants, where surface CO recovered to its normal level in China on around the 34th day after the Lunar New Year, while surface SO2 and NO2 rebounded more than 2 times slower due to more CO emissions from residents' increased indoor cooking and atmospheric oxidation capacity. Surface NO2, SO2, and CO reached their peak annual concentrations of 21.3 ± 8.8 µg m-3, 23.1 ± 13.3 µg m-3, and 1.01 ± 0.29 mg m-3 in 2013, then continuously declined over time by 12 %, 55 %, and 17 %, respectively, until 2020. The declining rates were more prominent from 2013 to 2017 due to the sharper reductions in anthropogenic emissions but have slowed down in recent years. Nevertheless, people still suffer from high-frequency risk exposure to surface NO2 in eastern China, while surface SO2 and CO have almost reached the World Health Organization (WHO) recommended short-term air quality guidelines (AQG) level since 2018, benefiting from the implemented stricter "ultra-low” emission standards. This reconstructed dataset of surface gaseous pollutants will benefit future (especially short-term) air pollution and environmental health-related studies.

Ground-Level NO2 Surveillance from Space Across China for High Resolution Using Interpretable Spatiotemporally Weighted Artificial Intelligence.

Nitrogen dioxide (NO2) at the ground level poses a serious threat to environmental quality and public health. This study developed a novel, artificial intelligence approach by integrating spatiotemporally weighted information into the missing extra-trees and deep forest models to first fill the satellite data gaps and increase data availability by 49% and then derive daily 1 km surface NO2 concentrations over mainland China with full spatial coverage (100%) for the period 2019-2020 by combining surface NO2 measurements, satellite tropospheric NO2 columns derived from TROPOMI and OMI, atmospheric reanalysis, and model simulations. Our daily surface NO2 estimates have an average out-of-sample (out-of-city) cross-validation coefficient of determination of 0.93 (0.71) and root-mean-square error of 4.89 (9.95) µg/m3. The daily seamless high-resolution and high-quality dataset "ChinaHighNO2" allows us to examine spatial patterns at fine scales such as the urban-rural contrast. We observed systematic large differences between urban and rural areas (28% on average) in surface NO2, especially in provincial capitals. Strong holiday effects were found, with average declines of 22 and 14% during the Spring Festival and the National Day in China, respectively. Unlike North America and Europe, there is little difference between weekdays and weekends (within ±1 µg/m3). During the COVID-19 pandemic, surface NO2 concentrations decreased considerably and then gradually returned to normal levels around the 72nd day after the Lunar New Year in China, which is about 3 weeks longer than the tropospheric NO2 column, implying that the former can better represent the changes in NOx emissions.

Opportunistic experiments to constrain aerosol effective radiative forcing.

Aerosol-cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide "opportunistic experiments" (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

Full-coverage mapping and spatiotemporal variations of ground-level ozone (O3) pollution from 2013 to 2020 across China

Ozone (O3) is an important trace and greenhouse gas in the atmosphere, posing a threat to the ecological environment and human health at the ground level. Large-scale and long-term studies of O3 pollution in China are few due to highly limited direct ground and satellite measurements. This study offers a new perspective to estimate ground-level O3 from solar radiation intensity and surface temperature by employing an extended ensemble learning of the space-time extremely randomized trees (STET) model, together with ground-based observations, remote sensing products, atmospheric reanalysis, and an emission inventory. A full-coverage (100%), high-resolution (10 km) and high-quality daily maximum 8-h average (MDA8) ground-level O3 dataset covering China (called ChinaHighO3) from 2013 to 2020 was generated. Our MDA8 O3 estimates (predictions) are reliable, with an average out-of-sample (out-of-station) coefficient of determination of 0.87 (0.80) and root-mean-square error of 17.10 (21.10) μg/m3 in China. The unique advantage of the full coverage of our dataset allowed us to accurately capture a short-term severe O3 pollution exposure event that took place from 23 April to 8 May in 2020. Also, a rapid increase and recovery of O3 concentrations associated with variations in anthropogenic emissions were seen during and after the COVID-19 lockdown, respectively. Trends in O3 concentration showed an average growth rate of 2.49 μg/m3/yr (p < 0.001) from 2013 to 2020, along with the continuous expansion of polluted areas exceeding the daily O3 standard (i.e., MDA8 O3 = 160 μg/m3). Summertime O3 concentrations and the probability of occurrence of daily O3 pollution have significantly increased since 2015, especially in the North China Plain and the main air pollution transmission belt (i.e., the “2 + 26” cities). However, a decline in both was seen in 2020, mainly due to the coordinated control of air pollution and ongoing COVID-19 effects. This carefully vetted and smoothed dataset is valuable for studies on air pollution and environmental health in China.

Abnormally Shallow Boundary Layer Associated With Severe Air Pollution During the COVID-19 Lockdown in China.

After the 2020 Lunar New Year, the Chinese government implemented a strict nationwide lockdown to inhibit the spread of the Coronavirus Disease 2019 (COVID-19). Despite the abrupt decreases in gaseous emissions caused by record-low anthropogenic activities, severe haze pollution occurred in northern China during the COVID lockdown. This paradox has attracted the attention of both the public and the scientific community. By analyzing comprehensive measurements of air pollutants, planetary boundary layer (PBL) height, and surface meteorology, we show that the severe air pollution episode over northern China coincided with the abnormally low PBL height, which had reduced by 45%, triggering strong aerosol-PBL interactions. After dynamical processes initiated the temperature inversion, the Beijing metropolitan area experienced a period with continuously shallow PBLs during the lockdown. This unprecedented event provided an experiment showcasing the role of meteorology, in particular aerosol-PBL interactions in affecting air quality.