Atmospheric Particle Hygroscopicity and the Influence by Oxidation State of Organic Aerosols in Urban Beijing.

A hygroscopic tandem differential mobility analyser (H-TDMA) was used to observe the size-resolved hygroscopic characteristics of submicron particles in January and April 2018 in urban Beijing. The probability distribution of the hygroscopic growth factor (HGF-PDF) in winter and spring usually showed a bimodal pattern, with more hygroscopic mode (MH) being more dominant. The seasonal variation in particle hygroscopicity was related to the origin of air mass, which received polluted southerly air masses in spring and clean northwesterly air masses in winter. Particles showed stronger hygroscopic behaviour during heavy pollution episodes (HPEs) with elevated concentrations of secondary aerosols, especially higher mass fraction of nitrate, which were indicated using the PM2.5 (particulate matter with diameter below 2.5 µm) mass concentration normalised by CO mass concentration. The hygroscopic parameter (κ) values were calculated using H-TDMA (κhtdma) and chemical composition (κchem). The closure study showed that κchem was overestimated in winter afternoon when compared with κhtdma, because the organic particle hygroscopic parameter (κorg) was overestimated in the calculations. It was influenced by the presence of a high concentration of hydrocarbon-like organic aerosol (HOA) with a weak water uptake ability. A positive relationship was observed between κorg and the ratio of oxygenated organic aerosol (OOA) and HOA, thereby indicating that the strong oxidation state enhanced the hygroscopicity of the particles. This study revealed the effect of local emission sources and secondary aerosol formation processes on particle hygroscopicity, which is of great significance for understanding the pollution formation mechanism in the North China Plain.

Modeling study on the roles of the deposition and transport of PM2.5 in air quality changes over central-eastern China.

The role of PM2.5 (particles with aerodynamic diameters ≤ 2.5 µm) deposition in air quality changes over China remains unclear. By using the three-year (2013, 2015, and 2017) simulation results of the WRF/CUACE v1.0 model from a previous work (Zhang et al., 2021), a non-linear relationship between the deposition of PM2.5 and anthropogenic emissions over central-eastern China in cold seasons as well as in different life stages of haze events was unraveled. PM2.5 deposition is spatially distributed differently from PM2.5 concentrations and anthropogenic emissions over China. The North China Plain (NCP) is typically characterized by higher anthropogenic emissions compared to southern China, such as the middle-low reaches of Yangtze River (MLYR), which includes parts of the Yangtze River Delta and the Midwest. However, PM2.5 deposition in the NCP is significantly lower than that in the MLYR region, suggesting that in addition to meteorology and emissions, lower deposition is another important factor in the increase in haze levels. Regional transport of pollution in central-eastern China acts as a moderator of pollution levels in different regions, for example by bringing pollution from the NCP to the MLYR region in cold seasons. It was found that in typical haze events the deposition flux of PM2.5 during the removal stages is substantially higher than that in accumulation stages, with most of the PM2.5 being transported southward and deposited to the MLYR and Sichuan Basin region, corresponding to a latitude range of about 24°N-31°N.

On the fossil and non-fossil fuel sources of carbonaceous aerosol with radiocarbon and AMS-PMF methods during winter hazy days in a rural area of North China plain.

Regional transport is a key source of carbonaceous aerosol in many Chinese megacities including Beijing. The sources of carbonaceous aerosol in urban areas have been studied extensively but are poorly known in upwind rural areas. This work aims to quantify the contributions of fossil and non-fossil fuel emissions to carbonaceous aerosols at a rural site in North China Plain in winter 2016. We integrated online high resolution-time of flight-aerosol mass spectrometer (HR-TOF-AMS) observations and radiocarbon (14C) measurements of fine particles with Positive Matrix Factorization (PMF) analysis as well as Extended Gelencsér (EG) method. We found that fine particle concentration is much higher at the rural site than in Beijing during the campaign (Dec 7, 2016 to Jan 8, 2017). PMF analysis of the AMS data showed that coal-combustion related organic aerosol (CCOA + Oxidized CCOA) and more oxidized oxygenated organic aerosol (MO-OOA) contributed 48% and 30% of organic matter to non-refractory PM1 (NR-PM1) mass. About 2/3 of the OC and EC were from fossil-fuel combustion. The EG method, combining AMS-PMF and 14C data, showed that primary and secondary OC from fossil fuel contribute 35% and 22% to total carbon (TC), coal combustion emission dominates the fossil fuel sources, and biomass burning accounted for 21% of carbonaceous aerosol. In summary, our results confirm that fossil fuel combustion was the dominant source of carbonaceous aerosol during heavy pollution events in the rural areas. Significant emissions of solid fuel carbonaceous aerosols at rural areas can affect air quality in downwind cities such as Beijing and Tianjin, highlighting the benefits of energy transition from solid fuels to cleaner energy in rural areas.

Intensified wintertime secondary inorganic aerosol formation during heavy haze pollution episodes (HPEs) in Beijing, China.

Air pollution in China is complex, and the formation mechanism of chemical components in particulate matter is still unclear. This study selected three consecutive heavy haze pollution episodes (HPEs) during winter in Beijing for continuous field observation, including an episode with heavy air pollution under red alert. Clean days during the observation period were selected for comparison. The HPE characteristics of Beijing in winter were: under the influence of adverse meteorological conditions such as high relative humidity, temperature inversion and low wind speed; and strengthening of secondary transformation reactions, which further intensified the accumulation of secondary aerosols and other pollutants, promoting the explosive growth of PM2.5. PM2.5/CO values, as indicators of the contribution of secondary transformation in PM2.5, were approximately 2 times higher in the HPEs than the average PM2.5/CO during the clean period. The secondary inorganic aerosols (sulfate nitrate and ammonium salt) were significantly enhanced during the HPEs, and the conversion coefficients were remarkably improved. In addition, it is interesting to observe that the production of sulfate tended to exceed that of nitrate in the late stage of all three HPEs. The existence of aqueous phase reactions led to the explosive growth sulfur oxidation ratio (SOR) and rapid generation of sulfate under high relative humidity (RH>70%).

Significant Changes in Chemistry of Fine Particles in Wintertime Beijing from 2007 to 2017: Impact of Clean Air Actions.

The Beijing government implemented a number of clean air action plans to improve air quality in the last 10 years, which contributed to changes in the concentration of fine particles and their compositions. However, quantifying the impacts of these interventions is challenging as meteorology masks the real changes in observed concentrations. Here, we applied a machine learning technique to decouple the effect of meteorology and evaluate the changes in the chemistry of nonrefractory PM1 (particulate matter less than 1 µm) in winter 2007, 2016, and 2017 as a result of the clean air actions. The observed mass concentrations of PM1 were 74.6, 90.2, and 36.1 µg m-3 in the three winters, while the deweathered concentrations were 74.2, 78.7, and 46.3 µg m-3, respectively. The deweathered concentrations of PM1, organics, sulfate, ammonium, chloride, SO2, NO2, and CO decreased by -38, -46, -59, -24, -51, -89, -16, and -52% in 2017 in comparison to 2007. On the contrary, the deweathered concentration of nitrates increased by 4%. Our results indicate that the clean air actions implemented in 2017 were highly effective in reducing ambient concentrations of SO2, CO, and PM1 organics, sulfate, ammonium, and chloride, but the control of nitrate and PM1 organics remains a major challenge.

Invert global and China's terrestrial carbon fluxes over 2019-2021 based on assimilating richer atmospheric CO2 observations.

With China's commitment to reach carbon peak by 2030 and achieve carbon neutrality by 2060, it is particularly important to obtain terrestrial ecosystem carbon fluxes with low uncertainty both globally and in China. The use of more observation data may help reduce the uncertainty of inverting carbon fluxes. This study uses the observation data from global stations, background stations and provincial stations in China, as well as the OCO-2 satellite, and uses the China Carbon Monitoring, Verification and Supporting System for Global (CCMVS-G) to estimate the carbon fluxes of global and Chinese terrestrial ecosystems from 2019 to 2021. The results revealed that the global terrestrial ecosystem carbon sink was approximately -3.40 Pg C/yr from 2019 to 2021. The carbon sinks in the Northern Hemisphere are large, especially in Asia, North America, and Europe. From 2019 to 2021, the carbon sink of China's terrestrial ecosystem was approximately -0.44 Pg C/yr. Carbon sinks exhibit significant seasonal and interannual variations in China. After assimilating the observation data, the uncertainty of the posterior flux is smaller than that of the prior flux, a more reasonable distribution of carbon sources and sinks can be obtained, and more accurate boundary conditions can be provided for the China Carbon Monitoring, Verification and Supporting System for Regional (CCMVS-R). In the future, it is important to establish a well-designed CO2 ground-based observation network.

Ongoing CO2 monitoring verify CO2 emissions and sinks in China during 2018-2021.

Accurate estimating CO2 emissions and sinks is crucial in achieving carbon neutrality in China. However, CO2 emissions from bottom-up inventories are uncertain at regional scales and lack independent verification from atmospheric perspectives. Here we integrated 39 high-precision CO2 stations in China to top-down invert emission-sink variations at 45 km × 45 km and achieved a full range of inventories verification. The results show that China's CO2 emissions are 15% higher than those of five bottom-up inventories, to an annual total of 3.40 Pg C a-1 for 2018-2021. After deducting human and livestock respiration, the annual CO2 emissions were 3.13 Pg C a-1 (11.48 Pg CO2 a-1). The annual increase in emissions slowed from 3.7% in 2019 to 1.1% in 2020 and resumed growth to 4.0% in 2021, consistent with observed CO2 growth rates in China. China's land CO2 sink, deducting farmland sinks and lateral fluxes, was 0.57 Pg C a-1 (2.09 Pg CO2 a-1) for 2018-2021 (higher than most global inverse models), accounting for ∼16.9% of anthropogenic CO2 emissions. The land sink in China decreased by -19.3% in 2019 due to a weak El Niño event and increased by 3.2% in 2020 and 13.7% in 2021. It is worth noting that inverse CO2 emissions and sinks in western China still face large uncertainty due to limited CO2 monitoring. Overall, our top-down estimates demonstrate spatiotemporal variations in CO2 emissions and sinks from atmospheric perspectives and highlight challenges for different provinces in achieving 2060 carbon neutrality with verified estimates.

Long-term trend of new particle formation events in the Yangtze River Delta, China and its influencing factors: 7-year dataset analysis.

To evaluate the influence of anthropogenic emission reductions since 2013 in China, a long-term trend analysis of the particle number size distribution (PNSD) and new particle formation (NPF) events in the Yangtze River Delta (YRD) region was conducted based on the PNSD measurement (diameter ranging from 3 to 850 nm) at the Lin'an (LAN) regional background station from 2013 to 2019. A modified Mann-Kendall test and a Theil-Sen estimator were used to calculate the overall trend of particle number concentrations in different modes and the relevant influencing factors. We observed a significant decreasing trend in the Aitken and accumulation mode number concentrations, with annual decrease rates of approximately 5.6% and 8.2%, respectively, resulting in an approximately 6.0% decline in total particles annually. However, the nucleation mode particle number concentration showed no significant trend from 2013 to 2016, but an increasing trend from 2016 to 2019, which was related to the NPF events occurrence frequency. The regional NPF events of "banana shape" accounted for an increasing fraction of all NPF events. As a key parameter influencing the NPF event, the condensation sink decreased by approximately 63% from 2013 to 2019. Moreover, the estimated sulfuric acid concentration decreased by approximately 50%, with a higher reduction rate occurring during 2013-2016 as result of the effective SO2 reduction. Surface meteorological factors (including the air temperature, relative humidity, air pressure, and wind) and the air masses origin were found to played minor roles in the long-term trend of NPF events. As PNSD and NPF events are closely related to changes in the particle emissions and regional air pollution levels, studies concerning PNSD and NPF are necessary to provide important information regarding air quality improvements and evaluating the efficacy of climate change mitigation strategies.

Effect of vegetation seasonal cycle alterations to aerosol dry deposition on PM2.5 concentrations in China.

The effect of vegetation seasonal cycle alterations to aerosol dry deposition on PM2.5 concentrations (hereafter referred as the VSC effect) in China was investigated using a numerical modelling system (WRF/CUACE). Two simulation experiments using the vegetation parameters in particle dry deposition schemes typical for January and July revealed an absolute increase in surface PM2.5 concentrations of about 2.4 µg/m3 and a 5.5% relative increase in China (within model domain 2). The effect in non-urban areas was more significant than that in urban areas. The increases in PM2.5 concentrations in Beijing-Tianjin-Hebei (BTH), Yangtze River Delta (YRD), Pearl River Delta (PRD), Sichuan Basin (SCB), and Central China (CC) were calculated as 1.9 µg/m3, 3.4 µg/m3, 3.1 µg/m3, 4.3 µg/m3, and 4.9 µg/m3, respectively, corresponding to relative increases of 2.9%, 4.5%, 5.4%, 5.8%, and 5.9%. These results demonstrate that the effect of decreased particle dry deposition due to reduced vegetation in southern areas was stronger, which was partially attributed to the increased vegetation cover and more significant seasonal changes in those regions. Furthermore, the increased PM2.5 concentrations caused by the VSC effect were transported from north to south via the winter northerly winds, which weakened the effect in North China Plain and enhanced the effect in parts of central and southern China, such as the south of CC. Although the surface PM2.5 concentration was relatively high in North China Plain, the effects of the northerly wind and relatively small dry deposition velocity meant that the removal of PM2.5 in that region was relatively less than in southern areas of China. These results will contribute to understanding of the underlying mechanisms of PM2.5 enhancement during winter in China.

Columnar optical, microphysical and radiative properties of the 2022 Hunga Tonga volcanic ash plumes.

The Hunga Tonga-Hunga Ha'apai eruption on January 15, 2022 was one of the most explosive volcanic eruptions of the 21st century and has attracted global attention. Here we show that large numbers of the volcanic aerosols from the eruption broke through the tropopause into the lower stratosphere, forming an ash plume with an overshooting top at 25-30 km altitude. In the four days following the eruption, the ash plume moved rapidly westward for nearly 10,000 km under stable stratospheric conditions characterized by strong tropical easterlies, weak meridional winds and weak vertical motion. The intrusion of the ash plume into the stratosphere resulted in a marked increase in atmospheric aerosol loading across northern Australia, with the aerosol optical depth (AOD) observed by satellites and sun-photometers peaking at 1.5 off the coast of northeastern Australia; these effects lasted for nearly three days. The ash plume was characterized by fine-mode particles clustered at a radius of about 0.26 µm, with an observed peak volume of 0.25 µm3 µm-2. The impact of the ash plume associated with the Hunga Tonga eruption on the stratospheric AOD and radiative balance in the tropical southern hemisphere is remarkable, with an observed volcanic-induced perturbation of the regional stratospheric AOD of up to 0.6. This perturbation largely explains an instantaneous bottom (top) of the atmosphere radiative forcing of -105.0 (-65.0) W m-2 on a regional scale.

The influence of stagnant and transport types weather on heavy pollution in the Yangtze-Huaihe valley, China.

The ambient atmospheric PM2.5 concentrations in Anhui Province, China, which links the Yangtze River Delta region, China's fastest growing economy area, with the Beijing-Tianjin-Hebei (BTH) region, China's most polluted region, are influenced not only by local emissions, but also by changes in regional circulation. During the period 2013-2017, when China adopted a series of pollution abatement measures, there were still occasional pollution episodes with significant increases in PM2.5 concentrations. PM2.5 rise instead during the period 2013-2017 in Anhui (the Center of the Yangtze-Huaihe, YH), when pollution emissions continued to decrease? What is the controlling mechanism behind these? By analyzing elements such as ground-based PM2.5 concentration and the planetary boundary layer (PBL) structure affecting it as well as larger scale circulation, combined with the analysis of a parameterized index, one can find that aerosol pollution in the YH region can usually be classified into three types. (1) There is a short-term transport stage (TS) in the initial stage of pollution, then as the pollutant concentrations increase, the PBL height decreases, the temperature inversion is gradually formed or strengthened, the wind speed decreases and the relative humidity of the lower layer increases, forming a two-way feedback mechanism in the cumulative stage (CS). (2) Pollutant concentrations will not drop rapidly in the later stage of CS, while a short-term TS will occur again. (3) The explosive rise (ER) events are mainly affected by transportation in the YH. The first of these types tends to be accompanied by the emergence and maintenance of heavy pollution periods (HPEs), and some phases is accompanied by explosive rises (ERs) in PM2.5 that at least double in a short period of time. To sum up, deterioration of meteorological conditions explaining approximately 68% to the increase in PM2.5 in the ER.

Seasonal variability and trends in global type-segregated aerosol optical depth as revealed by MISR satellite observations.

This study utilized a long-term (2001-2018) aerosol optical component dataset retrieved from the Multiangle Imaging Spectroradiometer (MISR), Version 23, to perform comprehensive analyses of the global climatology of seasonal AODs, partitioned by aerosol types (including small-size, medium-size, large-size, spherical, and non-spherical). By dividing eight different AOD bins and performing trend analysis, the seasonal variability and trends in these type-segregated AODs, as well as in the frequency occurrences (FOs) for different AOD bins, globally and over 12 regions of interest, were also investigated. In terms of particle size, small-size aerosol particles (diameter < 0.7 µm) contribute the largest to global extinction in all three seasons except winter. A similar globally dominant role is exhibited by spherical aerosols, which contribute 68.5%, 73.3%, 71.6% and 70.2% to the global total AOD (TAOD) in spring, summer, autumn and winter, respectively, on a global average scale. FOs with different aerosol loading levels suggested that the seasonal FOs tend to decrease progressively with increasing aerosol loading, except for Level 1 (TAOD< 0.05). Examination of the seasonal distribution of FOs revealed that the FO at Level 1 (Level 2, 0.05 < TAOD< 0.15) is much larger in summer/winter (winter/autumn) than in spring/autumn (spring/summer) over most areas of the world. However, the FOs for Level 3 (0.15 < TAOD< 0.25) to Level 8 (TAOD> 1.0) generally exhibit greater intensity in spring/summer than in autumn/winter. Temporal trend analyses showed that the seasonal TAOD experiences a significant decline during 2001-2018 in most regions globally, except in South Asia, the Middle East, and North Africa. Opposite seasonal trends in the above regions are closely related to the increase in FOs in the range of 0.4 < TAOD< 1.0. The global average TAOD shows the most pronounced decline in spring, falling by -10.4% (P < 0.05). Examination of the trends in type-segregated AODs further revealed that the decreases in size-segregated (shape-segregated) AODs all contribute to the decrease in seasonal TAOD, with small-size AOD (spherical AOD) contributing most significantly.

Robust prediction of hourly PM2.5 from meteorological data using LightGBM.

Retrieving historical fine particulate matter (PM2.5) data is key for evaluating the long-term impacts of PM2.5 on the environment, human health and climate change. Satellite-based aerosol optical depth has been used to estimate PM2.5, but estimations have largely been undermined by massive missing values, low sampling frequency and weak predictive capability. Here, using a novel feature engineering approach to incorporate spatial effects from meteorological data, we developed a robust LightGBM model that predicts PM2.5 at an unprecedented predictive capacity on hourly (R2 = 0.75), daily (R2 = 0.84), monthly (R2 = 0.88) and annual (R2 = 0.87) timescales. By taking advantage of spatial features, our model can also construct hourly gridded networks of PM2.5. This capability would be further enhanced if meteorological observations from regional stations were incorporated. Our results show that this model has great potential in reconstructing historical PM2.5 datasets and real-time gridded networks at high spatial-temporal resolutions. The resulting datasets can be assimilated into models to produce long-term re-analysis that incorporates interactions between aerosols and physical processes.

Drivers of the rapid rise and daily-based accumulation in PM1.

Submicron particle matter (PM1) that rapidly reaches exceedingly high levels in several or more hours in the North China Plain (NCP) has been threating~400 million individuals' health for decades. The precise cause of the rapid rise in PM1 remains uncertain. Based on sophisticated measurements in PM1 characterizations and corresponding boundary-layer (BL) meteorology in the NCP, it demonstrates that this rising is mainly driven by BL meteorological variability. Large increases in near-ground inversions and decreases in vertical heat/momentum fluxes during the day-night transition result in a significant reduction in mixing space. The PM1 that is vertically distributed before accumulates at the near-ground and then experiences a rapid rise. Besides meteorological variability, a part of the rise in organics is ascribed to an increase of coal combustion at midnight. The daily-based accumulation of PM1 is attributed to day-to-day vertical meteorological variability, particularly diminishing mixing layer height exacerbated by aerosol-radiation feedback. Resolved by a multiple linear regression model, BL meteorological variability can explain 71% variances of PM1. In contrast, secondary chemical reactions facilitate the daily-based accumulation of PM1 rather than the rapid rise. Our results show that BL meteorological variability plays a dominant role in PM1 rising and day-to-day accumulation, which is crucial for understanding the mechanism of heavy pollution formation.

Evaluating the contributions of changed meteorological conditions and emission to substantial reductions of PM2.5 concentration from 2016 to 2017 in Central and Eastern China.

The monthly average PM2.5 concentration decreased from 127.15 µg m-3 in December 2016 to 85.54 µg m-3 in December 2017 (approximately 33%) in Central and Eastern China (33°N-41°N, 113°E-118°E). This decrease is attributed to the combined impacts of meteorology and emission sources changes, though the question of which is more important has raised great concerns. Four sensitivity experiments based on the Global-Regional Assimilation and Prediction System coupled with the Chinese Unified Atmospheric Chemistry Environment (GRAPES-CUACE) model, together with comparative analysis of the observed meteorological conditions and emission inventory between 2016 and 2017, are used to evaluate the relative contributions of meteorology and emission to the substantial reductions of PM2.5 concentration from December 2016 to December 2017. The results show that the meteorological conditions and emission in December 2017 were both beneficial to the PM2.5 decrease in Central and Eastern China. Regarding the entire region, 21.9% of the PM2.5 decrease was a result of the favorable meteorological conditions, and 78.1% of the decrease was a result of emission reductions, showing the distinct contributions of emission reductions on the air quality. The relative contributions of meteorology varied from 12.2% to 50.9% to the PM2.5 decrease from December 2016 to December 2017, while the emission contributed 49.1% to 87.8%, in different cities depending on geographical location and topography. Meteorology showed the largest contributions to the PM2.5 decrease from 2016 to 2017 in Beijing (BJ), which caused the greatest total decrease of PM2.5 compared to that of other cities. In addition, in Central and Eastern China, the dominant factors of the decrease of PM2.5 were favorable meteorological conditions (accounting for 98.2%) during clear periods and emission reductions (accounting for 72.5-81.2%) during pollution periods.

Changes in ammonia and its effects on PM2.5 chemical property in three winter seasons in Beijing, China.

NH3, SO2, NOx and the inorganic ions of PM2.5 in winter 2009, 2014 and 2016 were examined to investigate the change in NH3 and aerosol chemistry in Beijing, China. NH3 concentrations showed an increase by 59% on average, in contrast to the decrease of SO2 by 63% from winter 2009 to 2016. The mean mass ratio of NH3/NHx was 0.83 ± 0.12 in 2016, which is higher than those obtained in 2009 and 2014, implying more NHx remaining as free NH3 in 2016 winter. Our findings suggest that vehicles exhaust emissions are an important NH3 source in urban central atmosphere of Beijing in winter. Despite the observed NOx presenting declining trends from 2014 to 2016, nitrate concentrations even exhibited a significant increasing trend, which may be largely attributable to high NH3 levels. An in-depth analysis of measured NH3 and aerosol species in a heavy pollution episode in December 2016, combined with the acidity predicted by ISORROPIA II model demonstrated abundant NH3 most of the time in air, where NH3 is not only a precursor for NH4+ but also effect the neutralization of SO42- and NO3- in PM2.5. With high RH and low photochemical activity, elevated NO3- concentration was attributed to an enhanced heterogeneous conversion of NOx to HNO3 to form NH4NO3 in pollution transport stage. The decrease in NOx from high level and the increase in NH3, with peaks of SO42- occurring were observed in pollution cumulative stage. The aqueous-phase oxidation of SO2 by NO2 to sulfate might play an important role with high pH values. Our results suggested that the simultaneous control of NH3 emissions in conjunction with SO2 and NOx emissions would be more effective in reducing particulate matter PM2.5 formation.

Relatively weak meteorological feedback effect on PM2.5 mass change in 2017/18 in the Beijing area: Observational evidence and machine-learning estimations.

Heavy aerosol pollution episodes (HPEs) in Beijing are worsened by the two-way feedback mechanism between unfavorable meteorological conditions and cumulative aerosols. In Winter 2017/18, mean PM2.5 mass concentration substantially decreased by 62% from 113 µg m-3 in Winter 2016/17 to 43 µg m-3. With reduced PM2.5 levels, the meteorological feedback on PM2.5 was relatively weak in Winter 2017/18. However, the weakening degree and its contributions to PM2.5 reduction are still uncertain. In this study, we investigated the change in the aerosol-induced modification of atmospheric stratification by combining PM2.5 data, radiosonde observations, and ERA-Interim reanalysis data, and then estimated the weakened meteorological feedback effect on PM2.5 change using machine learning. During polluted days, near-ground cooling bias, specific humidity (SH) increase, and relative humidity (RH) enhancement in Winter 2017/18 merely account for 38%, 65%, and 36% of the meteorological modification caused by aerosols in Winter 2016/17, respectively. Using machine learning algorithms with three most related variables, we found that during polluted days, the PM2.5 increase due to the meteorological feedback in Winter 2017/18 was merely 49% of that in Winter 2016/17. Effective pollution control and more favorable meteorological conditions have resulted in an additional benefit in PM2.5 reduction.

The effects of the "two-way feedback mechanism" on the maintenance of persistent heavy aerosol pollution over areas with relatively light aerosol pollution in northwest China.

Persistent heavy aerosol pollution episodes (HPEs) often occur in the central and eastern regions of China during the wintertime. When PM2.5 mass concentration cumulates to a certain extent that normally exceeds 100 µg m-3, the PM2.5 pollution will then further worsen the meteorological conditions in boundary layer (BL), resulting in significant two-way feedback between the cumulative PM2.5 pollution and worsened meteorological conditions. In the less polluted northwest area of China, whether there is significant two-way feedback phenomenon mentioned above after the accumulation of PM2.5 mass concentration has always been an issue of concern for understanding the full picture of meteorological causes of HPEs in China. Here, measurements of PM2.5 concentration, meteorological data and an integrated pollution-linked meteorological index (PLAM) are used to characterize the relationship between meteorological elements and PM2.5 concentration in persistent HPEs from 1 December 2016 to 10 January 2017 in Lanzhou and Urumqi. In early stage of the HPEs formation, the general 500 hPa circulation situations are normally high-pressure ridge or zonal westerly airflow patterns, associating with worsened meteorological conditions. At this time, with the decrease of BL height, the mass concentration of PM2.5 also increases as the pollutants mix in a relatively small space as compared to the clean period. When PM2.5 cumulates to a certain extent (above 75 µg m-3 in Lanzhou and above 100 µg m-3 in Urumqi), there are often obvious inversion and humidification in the near-surface. The inversion is mainly caused by the accumulation of the PM2.5 concentration, which indicates that even in northwest China, where anthropogenic activities are less affected and PM2.5 pollution is less serious, the cumulative PM2.5 can nonetheless worsen meteorological conditions. The worsened meteorological conditions, which are quantified by the PLAM index, dominate the changes in PM2.5 in the explosive growth of persistent HPEs (accounted for 50-85%).

Observational study of aerosol hygroscopic growth on scattering coefficient in Beijing: A case study in March of 2018.

A humidified nephelometer system was deployed to measure the aerosol scattering coefficients at RH < 30% and RH in the range of 40 to 85% simultaneously in megacity Beijing in March 2018. The aerosol optical properties and aerosol hygroscopicity of two sizes (PM10 and PM1) during the pollution period, dust period and a new particle formation event (NPF) were analyzed. During the pollution period, the scattering and absorption coefficients increased dramatically with the accumulation of pollutants, while scattering Ångström exponent (SAE), submicron scattering fraction (Rsp), submicron absorption fraction (Rap) decreased, as well as single scattering albedo (SSA) rose slightly, which indicated the increasing contribution of larger particle to scattering and absorption, and enhanced the scattering ability of aerosols. The average PM10 mass scattering efficiency is 3.86 ±â€¯1.19 m2 g-1 with a range of 2.05-5.74 m2 g-1 during the pollution period, and 0.40 ±â€¯0.05 m2 g-1 during the dust period. Rsp at wavelength of 550 nm varied from 55.8% to 89.3% during the measurement period, with the average of 64.8% ±â€¯5.2% and 73.1% ±â€¯6.8% during the pollution period and dust period, respectively, which suggests that the aerosol scattering coefficient is mainly affected by fine particles. The average PM10 and PM1 aerosol scattering hygroscopic growth factors f(80%) are 1.75 ±â€¯0.05 and 1.75 ±â€¯0.04 during the pollution period, 1.14 ±â€¯0.09 and 1.15 ±â€¯0.06 during the dust period, 1.59 ±â€¯0.05 and 1.60 ±â€¯0.06 during the NPF event period, respectively. Aerosol scattering hygroscopic growth factors showed a strong correlation with the scattering Ångström exponent which suggests the hygroscopicity is much stronger for fine particles (SAE > 1.5) than the coarse particles (SAE < 1.0).

Interdecadal changes of summer aerosol pollution in the Yangtze River Basin of China, the relative influence of meteorological conditions and the relation to climate change.

Winter is a season of much concern for aerosol pollution in China, but less concern for pollution in the summertime. There are even less concern and larger uncertainty about interdecadal changes in summer aerosol pollution, relative influence of meteorological conditions, and their links to climate change. Here we try to reveal the relation among interdecadal changes in summer's most important circulation system affecting China (East Asian Summer Monsoon-EASM), an index of meteorological conditions (called PLAM, Parameter Linking Air Quality and Meteorological Elements, which is almost linearly related with aerosol pollution), and aerosol optical depth (AOD) in the middle and lower reaches of the Yangtze River (M-LYR) in central eastern China during summertime since the 1960's. During the weak monsoon years, the aerosol pollution load was heavier in the M-LYR and opposite in the strong monsoon years mainly influenced by EASM and associated maintenance position of the anti-Hadley cell around 115°E. The interdecadal changes in meteorological conditions and their associated aerosol pollution in the context of such climate change have experienced four periods since the 1960's, which were a relatively large decreased period from 1961 to 1980, a large rise between 1980 and 1999, a period of slow rise or maintenance from 1999 to 2006, and a relatively rapid rise between 2006 and 2014. Among later three pollution increased periods, about 51%, 25% and 60% of the aerosol pollution change respectively come from the contribution of worsening weather conditions, which are found to be greatly affected by changes in EASM.