Vertical Evolution of Ozone Formation Sensitivity Based on Synchronous Vertical Observations of Ozone and Proxies for Its Precursors: Implications for Ozone Pollution Prevention Strategies.

Photochemical ozone (O3) formation in the atmospheric boundary layer occurs at both the surface and elevated altitudes. Therefore, the O3 formation sensitivity is needed to be evaluated at different altitudes before formulating an effective O3 pollution prevention and control strategy. Herein, we explore the vertical evolution of O3 formation sensitivity via synchronous observations of the vertical profiles of O3 and proxies for its precursors, formaldehyde (HCHO) and nitrogen dioxide (NO2), using multi-axis differential optical absorption spectroscopy (MAX-DOAS) in urban areas of the Beijing-Tianjin-Hebei (BTH), Yangtze River Delta (YRD), and Pearl River Delta (PRD) regions in China. The sensitivity thresholds indicated by the HCHO/NO2 ratio (FNR) varied with altitude. The VOC-limited regime dominated at the ground level, whereas the contribution of the NOx-limited regime increased with altitude, particularly on heavily polluted days. The NOx-limited and transition regimes played more important roles throughout the entire boundary layer than at the surface. The feasibility of extreme NOx reduction to mitigate the extent of the O3 pollution was evaluated using the FNR-O3 curve. Based on the surface sensitivity, the critical NOx reduction percentage for the transition from a VOC-limited to a NOx-limited regime is 45-72%, which will decrease to 27-61% when vertical evolution is considered. With the combined effects of clean air action and carbon neutrality, O3 pollution in the YRD and PRD regions will transition to the NOx-limited regime before 2030 and be mitigated with further NOx reduction.

Satellite spectroscopy reveals the atmospheric consequences of the 2022 Russia-Ukraine war.

With increasing geopolitical conflicts and climate change, the effects of war on the atmosphere remain unclear, especially the recent large-scale war between Russia and Ukraine. Here, we assess how war affects human emission activities by observing atmospheric nitrogen dioxide (NO2) using high-resolution satellite spectroscopy. Spatial and temporal responses of atmospheric composition to armed conflict are characterized. Significant decreases in NO2 concentrations of 10.7-27.3 % occurred in most Ukrainian cities at the beginning of the war, in contrast to dramatic increases in NO2 concentrations in Russian cities outside the northern border. Anomalous changes in NO2 were also found in transportation hubs. By excluding the effect of meteorology, the machine learning model indicates that war-induced changes in anthropogenic emissions may account for ∼40 % of the reduction in NO2 pollution for major cities such as Kyiv. Our study demonstrates that satellites can provide a unique perspective on the atmospheric consequences of humanitarian disasters.

Progress in quantitative research on the relationship between atmospheric oxidation and air quality.

Atmospheric oxidizing capacity (AOC) is an essential driving force of troposphere chemistry and self-cleaning, but the definition of AOC and its quantitative representation remain uncertain. Driven by national demand for air pollution control in recent years, Chinese scholars have carried out studies on theories of atmospheric chemistry and have made considerable progress in AOC research. This paper will give a brief review of these developments. First, AOC indexes were established that represent apparent atmospheric oxidizing ability (AOIe) and potential atmospheric oxidizing ability (AOIp) based on aspects of macrothermodynamics and microdynamics, respectively. A closed study refined the quantitative contributions of heterogeneous chemistry to AOC in Beijing, and these AOC methods were further applied in Beijing-Tianjin-Hebei and key areas across the country. In addition, the detection of ground or vertical profiles for atmospheric OH·, HO2·, NO3· radicals and reservoir molecules can now be obtained with domestic instruments in diverse environments. Moreover, laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O3 and NO2, which are typical oxidants in the surface/interface atmosphere, and the evolutionary and budgetary implications of atmospheric oxidants reacting under multispecies, multiphase and multi-interface conditions were obtained. Finally, based on the GRAPES-CUACE adjoint model improved by Chinese scholars, simulations of key substances affecting atmospheric oxidation and secondary organic and inorganic aerosol formation have been optimized. Normalized numerical simulations of AOIe and AOIp were performed, and regional coordination of AOC was adjusted. An optimized plan for controlling O3 and PM2.5 was analyzed by scenario simulation.

Identification of volatile organic compound emissions from anthropogenic and biogenic sources based on satellite observation of formaldehyde and glyoxal.

Anthropogenic volatile organic compounds (VOCs) are serious pollutants in the atmosphere because of their toxicity and as precursors of secondary organic aerosols and ozone pollution. Although in-situ measurements provide accurate information on VOCs, their spatial coverage is limited and insufficient. In this study, we provide a global perspective for identifying anthropogenic VOC emission sources through the ratio of glyoxal to formaldehyde (RGF) based on satellite observations. We assessed typical cities and polluted areas in the mid latitudes and found that some Asian cities had higher anthropogenic VOC emissions than cities in Europe and America. For heavily polluted areas, such as the Yangtze River Delta (YRD), the areas dominated by anthropogenic VOCs accounted for 23 % of the total study areas. During the COVID-19 pandemic, a significant decline in RGF values was observed in the YRD and western United States, corresponding to a reduction in anthropogenic VOC emissions. Furthermore, developing countries appeared to have higher anthropogenic VOC emissions than developed countries. These observations could contribute to optimising industrial structures and setting stricter pollution standards to reduce anthropogenic VOCs in developing countries.

Variability of PM2.5 and O3 concentrations and their driving forces over Chinese megacities during 2018-2020.

Recently, air pollution especially fine particulate matters (PM2.5) and ozone (O3) has become a severe issue in China. In this study, we first characterized the temporal trends of PM2.5 and O3 for Beijing, Guangzhou, Shanghai, and Wuhan respectively during 2018-2020. The annual mean PM2.5 has decreased by 7.82%-33.92%, while O3 concentration showed insignificant variations by -6.77%-4.65% during 2018-2020. The generalized additive models (GAMs) were implemented to quantify the contribution of individual meteorological factors and their gas precursors on PM2.5 and O3. On a short-term perspective, GAMs modeling shows that the daily variability of PM2.5 concentration is largely related to the variation of precursor gases (R = 0.67-0.90), while meteorological conditions mainly affect the daily variability of O3 concentration (R = 0.65-0.80) during 2018-2020. The impact of COVID-19 lockdown on PM2.5 and O3 concentrations were also quantified by using GAMs. During the 2020 lockdown, PM2.5 decreased significantly for these megacities, yet the ozone concentration showed an increasing trend compared to 2019. The GAMs analysis indicated that the contribution of precursor gases to PM2.5 and O3 changes is 3-8 times higher than that of meteorological factors. In general, GAMs modeling on air quality is helpful to the understanding and control of PM2.5 and O3 pollution in China.

Inferring global surface HCHO concentrations from multisource hyperspectral satellites and their application to HCHO-related global cancer burden estimation.

Formaldehyde (HCHO) is a toxic and hazardous air pollutant that widely exists in atmosphere. Insufficient spatial and temporal coverage of surface HCHO measurements is limiting studies on surface HCHO-related air quality management and health risk assessment. This study develops a method to derive global ground-level HCHO concentrations from satellite-based tropospheric HCHO columns using TM5-simulated surface-to-column conversion factor with coarse spatial resolution. The method improves the factor more representative in finer grids by constraining TM5-simulated vertical profile shapes with satellite HCHO columns. The surface HCHO concentrations derived by the Ozone Mapping and Profiler Suite (OMPS) show good correlation with in situ HCHO measurements (R = 0.59) from the U.S. Environmental Protection Agency surface network. We investigated how surface HCHO relates to urbanization and population aggregation over seven regions with high HCHO pollution. The results show urban HCHO increases as a power function with population size in China, India, and West Asia. HCHO concentrations in rural aeras also present strong log-log relationship with population aggregation in China, India, the United States, and Europe. Moreover, OMPS-derived ground-level HCHO concentrations were used to estimate global cancer burden caused by long-term outdoor HCHO exposure. The results show that up to 418188 more people worldwide will develop this cancer during the human life cycle. The global cancer burden is mainly from the South-East Asia region (33.11 %) and the Western Pacific region (22.95 %). This cancer occurrence in India and China is ranked 1st and 2nd in the world due to the large population size and serious HCHO pollution. Besides, global surface HCHO concentrations and cancer burden derived from the Environmental Trace Gases Monitoring Instrument which is China's first hyperspectral space-based spectrometer are found similar patterns with that from OMPS. Our results provide new insight into the impact of population urbanization on HCHO pollution and global outdoor HCHO-caused health risks.

Observations of atmospheric CO2 and CO based on in-situ and ground-based remote sensing measurements at Hefei site, China.

The characteristics of long time series of CO2 and CO surface concentrations, tropospheric and total column dry-air mole fractions (DMF) from May 2015 to December 2019 were investigated. Both CO2 and CO show different seasonality for the three datasets. The annual increasing trend of CO2 is similar for all three datasets. However, the annual decreasing trend of CO for surface concentration is high compared to the other two measurements, mainly due to the improved combustion efficiency from power generation in recent years. The correlation between the tropospheric and total atmospheric CO2 and CO is higher than that between the surface concentration and tropospheric CO2 and CO. This is because the tropospheric and total atmospheric results both have common vertical profiles for CO2 and CO respective mole fractions that were observed in troposphere. Furthermore, the enhancement ratios of CO2 to CO derived from the three datasets during the period from 2016 to 2019 were compared. The ratio of ∆CO2 to ∆CO has an obvious increase with altitude each year, which means that the combustion efficiencies obtained from the three datasets are different. All ratios for the three datasets showed a slight increasing trend in recent years, which is attributed to increased combustion efficiency due to governmental measures for energy savings and emission reductions.

Vertical profiles of the transport fluxes of aerosol and its precursors between Beijing and its southwest cities.

The influence of regional transport on aerosol pollution has been explored in previous studies based on numerical simulation or surface observation. Nevertheless, owing to inhomogeneous vertical distribution of air pollutants, vertical observations should be conducted for a comprehensive understanding of regional transport. Here we obtained the vertical profiles of aerosol and its precursors using ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) at the Nancheng site in suburban Beijing on the southwest transport pathway of the Beijing-Tianjin-Hebei (BTH) region, China, and then estimated the vertical profiles of transport fluxes in the southwest-northeast direction. The maximum net transport fluxes per unit cross-sectional area, calculated as pollutant concentration multiply by wind speed, of aerosol extinction coefficient (AEC), NO2, SO2 and HCHO were 0.98 km-1 m s-1, 24, 14 and 8.0 µg m-2 s-1 from southwest to northeast, which occurred in the 200-300 m, 100-200 m, 500-600 m and 500-600 m layers, respectively, due to much higher pollutant concentrations during southwest transport than during northeast transport in these layers. The average net column transport fluxes were 1200 km-1 m2 s-1, 38, 26 and 15 mg m-1 s-1 from southwest to northeast for AEC, NO2, SO2 and HCHO, respectively, in which the fluxes in the surface layer (0-100 m) accounted for only 2.3%-4.2%. Evaluation only based on surface observation would underestimate the influence of the transport from southwest cities to Beijing. Northeast or weak southwest transports dominated in clean conditions with PM2.5 <75 µg m-3 and intense southwest transport dominated in polluted conditions with PM2.5 >75 µg m-3. Southwest transport through the middle boundary layer was a trigger factor for aerosol pollution events in urban Beijing, because it not only directly bringing air pollutants, but also induced an inverse structure of aerosols, which resulted in stronger atmospheric stability and aggravated air pollution in urban Beijing.

Vertical distributions and potential sources of wintertime atmospheric pollutants and the corresponding ozone production on the coast of Bohai Sea.

This study investigated the wintertime vertical distributions and source areas of aerosols, NO2, and HCHO in a coastal city of Dongying from December 2020 to March 2021, using ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) and a potential source contribution function (PSCF) model, respectively. Moreover, the chemical production sensitivity of O3 at different height layers was analyzed using HCHO/NO2 ratios. The results revealed that the wintertime averaged highest concentrations of aerosol (1.25 km-1), NO2 (14.81 ppb), and HCHO (2.32 ppb) were mainly distributed at the surface layer, 100-200 m layer, and 200-300 m layer, respectively. Regarding the diurnal cycles, high concentrations of aerosol (>1.4 km-1) and NO2 (>16.0 ppb) usually appeared in the early morning and late afternoon, while high concentrations of HCHO (>2.5 ppb) usually occurred during 12:00-15:00. The PSCF model revealed that the wintertime aerosol mainly originated from Shandong, northern Jiangsu, Korea, and the northwestern Mongolian Plateau. Below 200 m, NO2 was mainly from western Shandong, whereas above 600 m, it was mainly from northern Shandong and the Beijing-Tianjin-Hebei (BTH) region. The corresponding sources for HCHO were central and southern Shandong (below 200 m) and northern Shandong, northern Jiangsu, and southeastern BTH (above 600 m). In addition, the chemical production sensitivity of O3 below 100 m was observed only in the VOC-limited regime. The percentages of O3 production under the NOx-limited, NOx-VOC-limited, and VOC-limited regimes were 10.75% (31.18%), 4.30% (19.35%), and 84.95% (49.47%) at the 500-600 m (900-1000 m) layer. This study has guiding significance for the coordinated control of PM2.5 and O3, and can assist in the implementation of regional joint prevention and control strategies for air pollutants.

Evolution of light absorption properties during photochemical aging of straw open burning aerosols.

Straw burning comprises more than 30% of all types of burned biomass in Asia, while the estimation of the emitted aerosols' direct radiative forcing effect suffers from large uncertainties, especially when atmospheric aging processes are considered. In this study, the light absorption properties of primary and aged straw burning aerosols in open fire were characterized at 7 wavelengths ranging from 370 nm to 950 nm in a chamber. The primary rice, corn and wheat straw burning bulk aerosols together had a mass absorption efficiency (MAE) of 2.43 ± 1.36 m2 g-1 at 520 nm and an absorption Ångström exponent (AAE) of 1.93 ± 0.71, while the primary sorghum straw burning bulk aerosols were characterized by a relatively lower MAE of 0.95 ± 0.54 m2 g-1 and a higher AAE of 4.80 ± 0.68. Both the MAE and AAE of primary aerosols can be well parameterized by the (PM-BC)/BC ratio (in wt.). The MAE of black carbon (BC) increased by 11-190% during photoreactions equivalent to 16-60 h of atmospheric aging, which was positively correlated with the (PM-BC)/(BC) ratio. The MAE of organic aerosols first slightly increased or leveled off, and then decreased. Specifically, at 370 nm, the first growth/plateau stage lasted until OH exposure reached 0.47-1.29 × 1011 molecule cm-3 s, and the following period exhibited decay rates of 1.0-2.8 × 10-12 cm3 molecule-1 s-1 against the OH radical, corresponding to half-lives of 46-134 h in a typical ambient condition. During photoreactions, competition among the lensing effect, growth/bleach of organic chromophores, and particle mass and size growth complicated the evolution of the direct radiative forcing effect. It is concluded that rice and corn straw burning aerosols maintained a warming effect after aging, while the cooling effect of fresh sorghum straw burning aerosols increased with aging.

Vertical distribution and temporal evolution of formaldehyde and glyoxal derived from MAX-DOAS observations: The indicative role of VOC sources.

Formaldehyde (HCHO) and glyoxal (CHOCHO) are important oxidization intermediates of most volatile organic compounds (VOCs), but their vertical evolution in urban areas is not well understood. Vertical profiles of HCHO, CHOCHO, and nitrogen dioxide (NO2) were retrieved from ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations in Hefei, China. HCHO and CHOCHO vertical profiles prefer to occur at higher altitudes compared to NO2, which might be caused by the photochemistry-oxidation of longer-lived VOCs at higher altitudes. Monthly means of HCHO concentrations were higher in summer, while enhanced amounts of NO2 were mainly observed in winter. CHOCHO exhibited a hump-like seasonal variation, with higher monthly-averaged values not only occurred in warm months (July-August) but also in cold months (November-December). Peak values mainly occurred during noon for HCHO but emerged in the morning for CHOCHO and NO2, suggesting that HCHO is stronger link to photochemistry than CHOCHO. We further use the glyoxal to formaldehyde ratio (GFR) to investigate the VOC sources at different altitudes. The lowest GFR value is almost found in the altitude from 0.2 to 0.4 km, and then rises rapidly as the altitude increases. The GFR results indicate that the largest contributor of the precursor VOC is biogenic VOCs at lower altitudes, while at higher altitudes is anthropogenic VOCs. Our findings provide a lot more insight into VOC sources at vertical direction, but more verification is recommended to be done in the future.

Inferring vertical variability and diurnal evolution of O3 formation sensitivity based on the vertical distribution of summertime HCHO and NO2 in Guangzhou, China.

The vertical distributions of formaldehyde (HCHO) and nitrogen dioxide (NO2) and their indicative roles in ozone (O3) sensitivity are important for designing O3 mitigation strategies. Using hyperspectral remote sensing observations, tropospheric vertical profiles of HCHO, NO2, and aerosol extinction were investigated in Guangzhou, China from July to September 2019. On both O3 non-exceedance and polluted days, the HCHO and aerosol vertical profiles exhibited similar Gaussian shapes, but the NO2 profile exhibited an exponential decreasing shape. HCHO and aerosol were especially sensitive to O3 pollution, with higher values generally occurring at approximately noon and late afternoon at higher altitudes. We attempted to study the diurnal evolution of O3 sensitivity at different altitudes based on the HCHO to NO2 ratio (FNR) vertical profile. The FNR thresholds marking the transition regime (2.5 < FNR < 4.0) were derived from the relationship between the increase in O3 (∆O3) and FNR. Our results showed that O3 sensitivity tends to be VOC-limited both at lower (below approximately 0.4 km) and higher (above approximately 1.8 km) altitudes throughout the daytime. In the middle altitudes, the photochemical formation of O3 was mainly in the transition/NOx-limited regime in the morning and afternoon but in the VOC-limited regime at noontime. The relationship between TROPOMI column FNR and near-surface O3 sensitivity was further investigated. Compared with the MAX-DOAS near-surface FNR, slightly higher values of column FNR would increase the number of days classified as transition regimes, which was mainly caused by the inhomogeneous vertical distribution of HCHO and NO2 in the lower troposphere. This study provides an improved understanding of vertical variability and diurnal evolution of O3 formation sensitivity.

First Chinese ultraviolet-visible hyperspectral satellite instrument implicating global air quality during the COVID-19 pandemic in early 2020.

In response to the COVID-19 pandemic, governments worldwide imposed lockdown measures in early 2020, resulting in notable reductions in air pollutant emissions. The changes in air quality during the pandemic have been investigated in numerous studies via satellite observations. Nevertheless, no relevant research has been gathered using Chinese satellite instruments, because the poor spectral quality makes it extremely difficult to retrieve data from the spectra of the Environmental Trace Gases Monitoring Instrument (EMI), the first Chinese satellite-based ultraviolet-visible spectrometer monitoring air pollutants. However, through a series of remote sensing algorithm optimizations from spectral calibration to retrieval, we successfully retrieved global gaseous pollutants, such as nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO), from EMI during the pandemic. The abrupt drop in NO2 successfully captured the time for each city when effective measures were implemented to prevent the spread of the pandemic, for example, in January 2020 in Chinese cities, February in Seoul, and March in Tokyo and various cities across Europe and America. Furthermore, significant decreases in HCHO in Wuhan, Shanghai, Guangzhou, and Seoul indicated that the majority of volatile organic compounds (VOCs) emissions were anthropogenic. Contrastingly, the lack of evident reduction in Beijing and New Delhi suggested dominant natural sources of VOCs. By comparing the relative variation of NO2 to gross domestic product (GDP), we found that the COVID-19 pandemic had more influence on the secondary industry in China, while on the primary and tertiary industries in Korea and the countries across Europe and America.

Impacts of TROPOMI-Derived NO X Emissions on NO2 and O3 Simulations in the NCP during COVID-19.

NO2 and O3 simulations have great uncertainties during the COVID-19 epidemic, but their biases and spatial distributions can be improved with NO2 assimilations. This study adopted two top-down NO X inversions and estimated their impacts on NO2 and O3 simulation for three periods: the normal operation period (P1), the epidemic lockdown period following the Spring Festival (P2), and back to work period (P3) in the North China Plain (NCP). Two TROPOspheric Monitoring Instrument (TROPOMI) NO2 retrievals came from the Royal Netherlands Meteorological Institute (KNMI) and the University of Science and Technology of China (USTC), respectively. Compared to the prior NO X emissions, the two TROPOMI posteriors greatly reduced the biases between simulations with in situ measurements (NO2 MREs: prior 85%, KNMI -27%, USTC -15%; O3 MREs: Prior -39%, KNMI 18%, USTC 11%). The NO X budgets from the USTC posterior were 17-31% higher than those from the KNMI one. Consequently, surface NO2 levels constrained by USTC-TROPOMI were 9-20% higher than those by the KNMI one, and O3 is 6-12% lower. Moreover, USTC posterior simulations showed more significant changes in adjacent periods (surface NO2: P2 vs P1, -46%, P3 vs P2, +25%; surface O3: P2 vs P1, +75%, P3 vs P2, +18%) than the KNMI one. For the transport flux in Beijing (BJ), the O3 flux differed by 5-6% between the two posteriori simulations, but the difference of NO2 flux between P2 and P3 was significant, where the USTC posterior NO2 flux was 1.5-2 times higher than the KNMI one. Overall, our results highlight the discrepancies in NO2 and O3 simulations constrained by two TROPOMI products and demonstrate that the USTC posterior has lower bias in the NCP during COVD-19.

Exploring the impact of new particle formation events on PM2.5 pollution during winter in the Yangtze River Delta, China.

New particle formation (NPF) events are an increasingly interesting topic in air quality and climate science. In this study, the particle number size distributions, and the frequency of NPF events over Hefei were investigated from November 2018 to February 2019. The proportions of the nucleation mode, Aitken mode, and accumulation mode were 24.59%, 53.10%, and 22.30%, respectively, which indicates the presence of abundant ultrafine particles in Hefei. Forty-six NPF events occurred during the observation days, accounting for 41.82% of the entire observation period. Moreover, the favorable meteorological conditions, potential precursor gases, and PM2.5 range of the NPF events were analyzed. Compared to non-NPF days, the NPF events preferentially occurred on days with lower relative humidity, higher wind speeds, and higher temperatures. When the PM2.5 was 15-20, 70-80, and 105-115 µg/m3, the frequency of the NPF events was higher. Nucleation mode particles were positively related to atmospheric oxidation indicated by ozone when PM2.5 ranged from 15 to 20 µg/m3, and related to gaseous precursors like SO2 and NO2 when PM2.5 was located at 70-80 and 105-115 µg/m3. On pollution days, NPF events did not directly contribute to the increase in the PM2.5 in the daytime, however, NPF events would occur during the night and the growth of particulate matter contributes to the nighttime PM2.5 contents. This could lead to pollution that lasted into the next day. These findings are significant to the improvement of our understanding of the effects of aerosols on air quality.

First global observation of tropospheric formaldehyde from Chinese GaoFen-5 satellite: Locating source of volatile organic compounds.

Satellite remote sensing is an important technique providing long-term and large-scale information of formaldehyde (HCHO), which plays a crucial role in atmospheric chemistry. Low signal-to-noise ratio and poor stability of the Environmental Trace Gases Monitoring Instrument (EMI) On board Gaofen-5 satellite, the first Chinese space-borne spectrometer, make HCHO retrieval extremely difficult. Here we firstly retrieved HCHO vertical column densities (VCDs) from EMI through in-flight spectral calibration, retrieval setting optimization and stripe correction. Retrieved EMI HCHO VCDs correlate well with those measured by Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) with normalize mean bias (NMB) below 25%. EMI HCHO VCDs are comparable with those observed by Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI). This study reveals that HCHO can be observed successfully by algorithm optimization despite of poor performance of space-borne spectrometer. The retrieved EMI HCHO VCDs are applied to locate emission sources of volatile organic compounds (VOCs).

Improved Anthropogenic SO2 Retrieval from High-Spatial-Resolution Satellite and its Application during the COVID-19 Pandemic.

Sulfur dioxide (SO2) measured by satellites is widely used to estimate anthropogenic emissions. The Sentinel-5 Precursor (S-5P) operational SO2 product is overestimated compared to the ground-based multiaxis differential optical absorption spectroscopy (MAX-DOAS) measurements in China and shows an opposite variation to the surface measurements, which limits the application of TROPOspheric monitoring instrument (TROPOMI) products in emissions research. Radiometric calibration, a priori profiles, and fitting windows might cause the overestimation of S-5P operational SO2 product. Here, we improve the optimal-estimation-based algorithm through several calibration methods. The improved retrieval agrees reasonably well with the ground-based measurements (R > 0.70, bias <13.7%) and has smaller biases (-28.9%) with surface measurements over China and India. It revealed that the SO2 column in March 2020 decreased by 51.6% compared to March 2019 due to the lockdown for curbing the spread of the COVID-19 pandemic, and there was a decrease of 50% during the lockdown than those after the lockdown, similar to the surface measurement trend, while S-5P operational SO2 product showed an unrealistic increase of 19%. In India, the improved retrieval identified obvious "hot spots" and observed a 30% decrease of SO2 columns during the lockdown.

Opposite impact of emission reduction during the COVID-19 lockdown period on the surface concentrations of PM2.5 and O3 in Wuhan, China.

To prevent the spread of the COVID-19 epidemic, the Chinese megacity Wuhan has taken emergent lockdown measures starting on January 23, 2020. This provided a natural experiment to investigate the response of air quality to such emission reductions. Here, we decoupled the influence of meteorological and non-meteorological factors on main air pollutants using generalized additive models (GAMs), driven by data from the China National Environmental Monitoring Center (CNEMC) network. During the lockdown period (Jan. 23 - Apr. 8, 2020), PM2.5, PM10, NO2, SO2, and CO concentrations decreased significantly by 45 %, 49 %, 56 %, 39 %, and 18 % compared with the corresponding period in 2015-2019, with contributions by S(meteos) of 15 %, 17 %, 13 %, 10 %, and 6 %. This indicates an emission reduction of NOx at least 43 %. However, O3 increased by 43 % with a contribution by S(meteos) of 6 %. In spite of the reduced volatile organic compound (VOC) emissions by 30 % during the strict lockdown period (Jan. 23 - Feb. 14, 2020), which likely reduced the production of O3, O3 concentrations increased due to a weakening of the titration effect of NO. Our results suggest that conventional emission reduction (NOx reduction only) measures may not be sufficient to reduce (or even lead to an increase of) surface O3 concentrations, even if reaching the limit, and VOC-specific measures should also be taken.

Vertical distributions of wintertime atmospheric nitrogenous compounds and the corresponding OH radicals production in Leshan, southwest China.

Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations were operated from 02 to 21 December 2018 in Leshan, southwest China, to measure HONO, NO2 and aerosol extinction vertical distributions, and these were the first MAX-DOAS measurement results in Sichuan Basin. During the measurement period, characteristic ranges for surface concentration were found to be 0.26-4.58 km-1 and averaged at 0.93 km-1 for aerosol extinction, 0.49 to 35.2 ppb and averaged at 4.57 ppb for NO2 and 0.03 to 7.38 ppb and averaged at 1.05 ppb for HONO. Moreover, vertical profiles of aerosol, NO2 and HONO were retrieved from MAX-DOAS measurements using the Heidelberg Profile (HEIPRO) algorithm. By analysing the vertical gradients of pollutants and meteorological information, we found that aerosol and HONO are strongly localised, while NO2 is mainly transmitted from the north direction (city center direction). Nitrogen oxides such as HONO and NO2 are important for the production of hydroxyl radical (OH) and oxidative capacity in the troposphere. In this study, the averaged value of OH production rate from HONO is about 0.63 ppb/hr and maximum value of ratio between OH production from HONO and from (HONO+O3) is > 93% before12:00 in Leshan. In addition, combustion emission contributes to 26% for the source of HONO in Leshan, and we found that more NO2 being converted to HONO under the conditions with high aerosol extinction coefficient and high relative humidity is also a dominant factor for the secondary produce of HONO.

Characteristic analysis of continuous new particle formation events in Hefei: A case study of the May Day holiday in China.

Studying the characteristics of new particle formation (NPF) is conducive to exploring the impact of atmospheric particulate matter on the climate, environment, and human health. The particle number size distributions (5.6-560 nm) of aerosols were measured using a fast mobility particle sizer (FMPS) from 1 to 11 May 2019. The clean atmosphere was one of the basic conditions for the occurrence of this continuous new particle formation events. It started between 9:00 and 12:00, and it mainly ended after 20:00. The growth rate (GR) and condensation sink (CS) values in Hefei were 2.98 ± 0.97 nm·h-1 and (3.0 ± 0.4) × 10-2 s-1, respectively. Back trajectory clustering analysis revealed that the mass concentration of the air masses from the southeastern part of Henan Province and the southern part of Anhui Province surrounding the study area were relatively high. The analysis results of the potential source contribution function (PSCF) and the concentration weighted trajectory (CWT) methods show that in addition to local pollution, the long-distance transport of pollutants in the Yangtze River Delta (YRD) greatly contributed to the accumulation modal particulate concentration in Hefei. Moreover, the population affected by PM2.5 during the observation period reached 8.19 × 104, accounting for 1.08% to the total population in Hefei. The premature death cases associated with PM2.5 reached 8.35 × 102. This study is helpful to understand the main influencing factors of consecutive NPF events and the health risks of fine particles.