East Asian winter monsoon intensification over the Northwest Pacific Ocean driven by late Miocene atmospheric CO2 decline.

East Asian winter monsoon (EAWM) activity has had profound effects on environmental change throughout East Asia and the western Pacific. Much attention has been paid to Quaternary EAWM evolution, while long-term EAWM fluctuation characteristics and drivers remain unclear, particularly during the late Miocene when marked global climate and Asian paleogeographic changes occurred. To clarify understanding of late Miocene EAWM evolution, we developed a high-precision 9-million-year-long stacked EAWM record from Northwest Pacific Ocean abyssal sediments based on environmental magnetism, sedimentology, and geochemistry, which reveals a strengthened late Miocene EAWM. Our paleoclimate simulations also indicate that atmospheric CO2 decline played a vital role in this EAWM intensification over the Northwest Pacific Ocean compared to other factors, including central Asian orogenic belt and northeastern Tibetan Plateau uplift and Antarctic ice-sheet expansion. Our results expand understanding of EAWM evolution from inland areas to the open ocean and indicate the importance of atmospheric CO2 fluctuations on past EAWM variability over large spatial scales.

Climate change impacts on the extreme power shortage events of wind-solar supply systems worldwide during 1980-2022.

Economic productivity depends on reliable access to electricity, but the extreme shortage events of variable wind-solar systems may be strongly affected by climate change. Here, hourly reanalysis climatological data are leveraged to examine historical trends in defined extreme shortage events worldwide. We find uptrends in extreme shortage events regardless of their frequency, duration, and intensity since 1980. For instance, duration of extreme low-reliability events worldwide has increased by 4.1 hours (0.392 hours per year on average) between 1980-2000 and 2001-2022. However, such ascending trends are unevenly distributed worldwide, with a greater variability in low- and middle-latitude developing countries. This uptrend in extreme shortage events is driven by extremely low wind speed and solar radiation, particularly compound wind and solar drought, which however are strongly disproportionated. Only average 12.5% change in compound extremely low wind speed and solar radiation events may give rise to over 30% variability in extreme shortage events, despite a mere average 1.0% change in average wind speed and solar radiation. Our findings underline that wind-solar systems will probably suffer from weakened power security if such uptrends persist in a warmer future.

The multi-year contribution of Indo-China peninsula fire emissions to aerosol radiation forcing in southern China during 2013-2019.

Fire emissions in Southeast Asia transported to southern China every spring (March-May), influencing not only the air quality but also the weather and climate. However, the multi-year variations and magnitude of this impact on aerosol radiation forcing in southern China remain unclear. Here, we quantified the multi-year contributions of fire emissions in Indo-China Peninsula (ICP) region to aerosol radiation forcing in the various southern Chinese provinces during the fire season (March-May) of 2013-2019 combining the 3-dimension chemical transport model and the Column Radiation Model (CRM) simulations. The models' evaluations showed they reasonably capture the temporal and spatial distribution of surface aerosol concentrations and column aerosol optical properties over the study regions. The fire emissions over the ICP region were found to increase the aerosol optical depth (AOD) value by 0.1 (15 %) and reduce the single scattering albedo (SSA) in three southern regions of China (Yunnan-YN, Guangxi-GX, and Guangdong-GD from west to east), owing to increases in the proportions of black carbon (BC, 0.4 % ± 0.1 %) and organic carbon (OC, 3.0 % ± 0.9 %) within the aerosol compositions. The transported smoke aerosols cooled surface but heated the atmosphere in the southern China regions, with the largest mean reduction of -5 Wm-2 (-3 %) in surface shortwave radiation forcing and the maximum daily contributions of about -15 Wm-2 (-15 %) to the atmosphere radiation forcing in the GX region, followed by the GD and YN regions. The impacts of ICP fire emissions on aerosol optical and radiative parameters declined during 2013-2019, with the highest rate of 0.393 ± 0.478 Wm-2 yr-1 in the GX for the shortwave radiation forcing in the atmosphere. Besides, their yearly changes in the contribution were consistent with the annual fire emissions in the ICP region. Such strong radiative perturbations of ICP fire emissions were expected to influence regional meteorology in southern China and should be considered in the climate simulations.

Aerosol forcing regulating recent decadal change of summer water vapor budget over the Tibetan Plateau.

The Tibetan Plateau (TP), known as the Asian water tower, has been getting wetter since the 1970s. However, the primary drivers behind this phenomenon are still highly controversial. Here, we isolate the impacts of greenhouse gases (GHG), aerosols, natural forcings and internal climate variability on the decadal change of summer water vapor budget (WVB) over the TP using multi-model ensemble simulations. We show that an anomalous Rossby wave train in the upper troposphere travelling eastward from central Europe and equatorward temperature gradient in eastern China due to the inhomogeneous aerosol forcing in Eurasia jointly contribute to anomalous easterly winds over the eastern TP. Such anomalous easterly winds result in a significant decrease in water vapor export from the eastern boundary of the TP and dominate the enhanced summer WVB over the TP during 1979-2014. Our results highlight that spatial variation of aerosol forcing can be used as an important indicator to project future WVB over the TP.

Columnar optical-radiative properties and components of aerosols in the Arctic summer from long-term AERONET measurements.

Aerosols as an external factor have an important role in the amplification of Arctic warming, yet the geography of this harsh region has led to a paucity of observations, which has limited our understanding of the Arctic climate. We synthesized the latest decade (2010-2021) of data on the microphysical-optical-radiative properties of aerosols and their multi-component evolution during the Arctic summer, taking into consideration the important role of wildfire burning. Our results are based on continuous observations from eight AERONET sites across the Arctic region, together with a meteorological reanalysis dataset and satellite observations of fires, and utilize a back-trajectory model to track the source of the aerosols. The summer climatological characteristics within the Arctic Circle showed that the aerosols are mainly fine-mode aerosols (fraction >0.95) with a radius of 0.15-0.20 µm, a slight extinction ability (aerosol optical depth âˆ¼ 0.11) with strong scattering (single scattering albedo ∼0.95) and dominant forward scattering (asymmetry factor âˆ¼ 0.68). These optical properties result in significant cooling at the Earth's surface (∼-13 W m-2) and a weak cooling effect at the top of the atmosphere (∼-5 W m-2). Further, we found that Arctic region is severely impacted by wildfire burning events in July and August, which primarily occur in central and eastern Siberia and followed in subpolar North America. The plumes from wildfire transport aerosols to the Arctic atmosphere with the westerly circulation, leading to an increase in fine-mode aerosols containing large amounts of organic carbon, with fraction as high as 97-98 %. Absorptive carbonaceous aerosols also increase synergistically, which could convert the instantaneous direct aerosol radiative effect into a heating effect on the Earth-atmosphere system. This study provides insights into the complex sources of aerosol loading in the Arctic atmosphere in summer and emphasizes the important impacts of the increasingly frequent occurrence of wildfire burning events in recent years.

Evaluation of MERRA-2 and CAMS reanalysis for black carbon aerosol in China.

Black carbon (BC) constitutes a pivotal component of atmospheric aerosols, significantly impacting regional and global radiation balance, climate, and human health. In this study, we evaluated BC data in two prominent atmospheric composition reanalysis datasets: the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) and the Copernicus Atmosphere Monitoring Service (CAMS), and analyzed the causes of their deviations. This assessment is based on observational data collected from 34 monitoring stations across China from 2006 to 2022. Our research reveals a significant and consistent decline in BC concentrations within China, amounting to a reduction exceeding 67.33%. However, both MERRA-2 and CAMS reanalysis data fail to capture this declining trend. The average annual decrease of BC in MERRA-2 from 2006 to 2022 is only 0.06 µg/m3 per year, while the BC concentration in CAMS even increased with an average annual value of 0.014 µg/m3 per year. In 2022, MERRA-2 had overestimated BC concentration by 20% compared to observational data, while CAMS had overestimated it by approximately 66%. In the regional BC concentration analysis, the data quality of the reanalysis data is better in the South China (RM = 0.59, RC = 0.53), followed by the North China (RM = 0.50, RC = 0.42). Reanalysis BC data in Northwest China and the Tibetan Plateau are difficult to use for practical analysis due to their big difference with observation. In a comparison of the anthropogenic BC emissions inventory used in the two atmospheric composition reanalysis datasets with the Multi-resolution Emission Inventory model for Climate and air pollution research (MEIC) emissions inventory, we found that: Despite the significant decline in China's BC emissions, MERRA-2 still relies on the 2006 emissions inventory, while CAMS utilizes emission inventories that even show an increasing trend. These factors will undoubtedly lead to greater deviations between reanalysis and observational data.

Quantifying the contribution of local drivers to observed weakening of spring dust storm frequency over northern China (1982-2017).

Recent studies have suggested that spring dust storm (SDS) events in northern China (NC) have exhibited substantial decline over the past 30 years. However, it is unclear which local factors are most responsible for the decline in SDS events, and the contribution of each dominant factor remains to be determined. This study utilized high-density DS records and collocated homogenized surface meteorological observations from 1982 to 2017, in conjunction with land surface products, to examine the local drivers that influence the long-term variation in SDS frequency (SDSF) over the entire NC area and its three dust-source areas: northwestern China (NWC), north-central China (NCC), and northeastern China (NEC). Results indicated that the observed SDSF averaged over NC, NWC, NCC, and NEC has decreased by 144.4 %, 109.3 %, 166.4 %, and 92.2 %, respectively, during 1982-2017. The variation in SDSF is largely explained by variation in wind speed (WS), precipitation, volumetric soil moisture, and surface bareness. A multivariable linear regression model incorporating these local drivers accounted for 81.0 %, 74.0 %, and 46.9 % of the variance in SDSF in NWC, NCC, and NEC, respectively. Statistical analyses on the local drivers suggested that weakening of WS was the dominant factor in the reduction in SDSF over recent decades, contributing 76.9 %, 54.7 %, and 33.6 % of the variation in NWC, NCC, and NEC, respectively. More importantly, we revealed that the interannual variation in regional SDSF was not only controlled by local drivers, but also influenced by cross-regional transport of dust aerosols emitted from upstream source areas.

Recent Progress in Atmospheric Chemistry Research in China: Establishing a Theoretical Framework for the "Air Pollution Complex".

Atmospheric chemistry research has been growing rapidly in China in the last 25 years since the concept of the "air pollution complex" was first proposed by Professor Xiaoyan TANG in 1997. For papers published in 2021 on air pollution (only papers included in the Web of Science Core Collection database were considered), more than 24 000 papers were authored or co-authored by scientists working in China. In this paper, we review a limited number of representative and significant studies on atmospheric chemistry in China in the last few years, including studies on (1) sources and emission inventories, (2) atmospheric chemical processes, (3) interactions of air pollution with meteorology, weather and climate, (4) interactions between the biosphere and atmosphere, and (5) data assimilation. The intention was not to provide a complete review of all progress made in the last few years, but rather to serve as a starting point for learning more about atmospheric chemistry research in China. The advances reviewed in this paper have enabled a theoretical framework for the air pollution complex to be established, provided robust scientific support to highly successful air pollution control policies in China, and created great opportunities in education, training, and career development for many graduate students and young scientists. This paper further highlights that developing and low-income countries that are heavily affected by air pollution can benefit from these research advances, whilst at the same time acknowledging that many challenges and opportunities still remain in atmospheric chemistry research in China, to hopefully be addressed over the next few decades.

Unintended consequences of combating desertification in China.

Since the early 2000s, China has carried out extensive "grain-for-green" and grazing exclusion practices to combat desertification in the desertification-prone region (DPR). However, the environmental and socioeconomic impacts of these practices remain unclear. We quantify and compare the changes in fractional vegetation cover (FVC) with economic and population data in the DPR before and after the implementation of these environmental programmes. Here we show that climatic change and CO2 fertilization are relatively strong drivers of vegetation rehabilitation from 2001-2020 in the DPR, and the declines in the direct incomes of farmers and herders caused by ecological practices exceed the subsidies provided by governments. To minimize economic hardship, enhance food security, and improve the returns on policy investments in the DPR, China needs to adapt its environmental programmes to address the potential impacts of future climate change and create positive synergies to combat desertification and improve the economy in this region.

Description and evaluation of a newly developed emission inventory processing system (EMIPS).

Commonly available emission inventories are often incompatible with the input requirements of atmospheric chemistry models due to temporal and spatial resolution, pollutant types, etc. We present the Emission Inventory Processing System (EMIPS) version 1, an open-source and multi-scale atmospheric emission modeling framework that prepares specific emissions inputs for atmospheric chemistry models. EMIPS is a multifunctional and user-friendly system, coded in Jython and developed on the MeteoInfo software platform. It allows users to freely combine and process emission inventories to generate model-ready emissions data. The core functions of EMIPS include preprocessing, temporal allocation, spatial allocation, chemical speciation, and vertical allocation. We detail the implementation of each function in the body of this paper, and several examples are provided for illustration. The emission outputs obtained with EMIPS have been evaluated by simulating four pollutants (PM2.5, PM10, NO2, and O3) concentrations in January 2017 using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), and comparison of model results with the observations indicates the model can reproduce the temporal and spatial patterns of pollutants, suggesting that EMIPS is capable of supporting atmospheric chemistry modeling. We expect this work could help to improve air quality research and forecast.

Simultaneous profiling of dust aerosol mass concentration and optical properties with polarized high-spectral-resolution lidar.

Dust particles originating from arid desert regions can be transported over long distances, presenting severe risks to climate, environment, social economics, and human health at the source and downwind regions. However, there has been a dearth of continuous diurnal observations of vertically resolved mass concentration and optical properties of dust aerosols, which hinders our understanding of aerosol mixing, stratification, aerosol-cloud interactions, and their impacts on the environment. To fill the gap of the insufficient observations, to the best of our knowledge, this work presents the first high-spectral-resolution lidar (HSRL) observation providing days of continuous profiles of the mass concentration, along with particle linear depolarization ratio (PLDR), backscattering coefficient, extinction coefficient and lidar ratio (LR), simultaneously. We present the results of two strong dust events observed by HSRL over Beijing in 2021. The maximum particle mass concentrations reached (1.52 ± 3.5) x103 µg/m3 and (19.48 ± 0.36) x103 µg/m3 for the two dust events, respectively. The retrieved particle mass concentrations and aerosol optical depth (AOD) agree well with the observation from the surface PM10 concentrations and sun photometer with correlation coefficients of 0.90 and 0.95, respectively. The intensive properties of PLDR and LR of the dust aerosols are 0.31 ± 0.02 and 39 ± 7 sr at 532 nm, respectively, which are generally close to those obtained from observations in the downwind areas. Moreover, inspired by the observations from HSRL, a universal analytical relationship is discovered to evaluate the proportion of dust aerosol backscattering, extinction, AOD, and mass concentration using PLDR. The universal analytical relationship reveals that PLDR can directly quantify dust aerosol contribution, which is expected to further expand the application of polarization technology in dust detection. These valuable observations and findings further our understanding of the contribution of dust aerosol to the environment and help supplement dust aerosol databases.

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.

Changes in aerosol loading before, during and after the COVID-19 pandemic outbreak in China: Effects of anthropogenic and natural aerosol.

Anthropogenic emissions reduced sharply in the short-term during the coronavirus disease pandemic (COVID-19). As COVID-19 is still ongoing, changes in atmospheric aerosol loading over China and the factors of their variations remain unclear. In this study, we used multi-source satellite observations and reanalysis datasets to synergistically analyze the spring (February-May) evolution of aerosol optical depth (AOD) for multiple aerosol types over Eastern China (EC) before, during and after the COVID-19 lockdown period. Regional meteorological effects and the radiative response were also quantitatively assessed. Compared to the same period before COVID-19 (i.e., in 2019), a total decrease of -14.6 % in tropospheric TROPOMI nitrogen dioxide (NO2) and a decrease of -6.8 % in MODIS AOD were observed over EC during the lockdown period (i.e., in 2020). After the lockdown period (i.e., in 2021), anthropogenic emissions returned to previous levels and there was a slight increase (+2.3 %) in AOD over EC. Moreover, changes in aerosol loading have spatial differences. AOD decreased significantly in the North China Plain (-14.0 %, NCP) and Yangtze River Delta (-9.4 %) regions, where anthropogenic aerosol dominated the aerosol loading. Impacted by strong wildfires in Southeast Asia during the lockdown period, carbonaceous AOD increased by +9.1 % in South China, which partially offset the emission reductions. Extreme dust storms swept through the northern region in the period after COVID-19, with an increase of +23.5 % in NCP and + 42.9 % in Northeast China (NEC) for dust AOD. However, unfavorable meteorological conditions overwhelmed the benefits of emission reductions, resulting in a +20.1 % increase in AOD in NEC during the lockdown period. Furthermore, the downward shortwave radiative flux showed a positive anomaly due to the reduced aerosol loading in the atmosphere during the lockdown period. This study highlights that we can benefit from short-term controls for the improvement of air pollution, but we also need to seriously considered the cross-regional transport of natural aerosol and meteorological drivers.

Seasonal cycles and long-term trends of arctic tropospheric aerosols based on CALIPSO lidar observations.

Notable warming trends have been observed in the Arctic, with tropospheric aerosols being one of the key drivers. Here the seasonal cycles of three-dimensional (3D) distributions of aerosol extinction coefficients (AECs) and frequency of occurrences (FoOs) for different aerosol subtypes in the troposphere over the Arctic from 2007 to 2019 are characterized capitalizing on Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) Level-3 gridded aerosol profile product. Seasonal contributions of total and type-dependent aerosols through their partitioning within the planetary boundary layer (PBL) and free troposphere (FT) are also quantified utilizing the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) PBL height data. The results show substantial seasonal and geographical dependence in the distribution of aerosols over the Arctic. Sulfate, black carbon (BC), and organic carbon (OC) contribute most of the total AEC, with Eurasia being the largest contributor. The vertical structure of AECs and FoOs over the Arctic demonstrates that the vertical influence of aerosols is higher in eastern Siberia and North America than in northern Eurasia and its coasts. When the total aerosol optical depth (TAOD) is partitioned into the PBL and FT, results indicate that the contributions of TAOD within the FT tend to be more significant, especially in summer, with the FT contributes 64.2% and 69.2% of TAOD over the lower (i.e., 60° N-70° N) and high (i.e., north of 70° N) Arctic, respectively. Additionally, seasonal trend analyses suggest Arctic TAOD exhibits a multi-year negative trend in winter, spring, and autumn and a positive trend in summer during 2007-2019, due to an overall decrease in sulfate from weakened anthropogenic emissions and a significant increase in BC and OC from enhanced biomass burning activities. Overall, this study has potential implications for understanding the seasonal cycles and trends in Arctic aerosols.

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.

Water-soluble iron in PM2.5 in winter over six Chinese megacities: Distributions, sources, and environmental implications.

Water-soluble iron (ws-Fe) in PM2.5 plays a crucial role in biogeochemical cycles and atmospheric chemical processes. The anthropogenic sources of ws-Fe have attracted considerable attention owing to its high solubility. However, few studies have investigated the content of PM2.5 ws-Fe in the urban environment. In the present study, we characterized the spatial distributions of ws-Fe in six Chinese megacities in the winter of 2019. Furthermore, we investigated the speciation of PM2.5 ws-Fe (ws-Fe(II) and ws-Fe(III)), potential sources of ws-Fe, and association between ws-Fe and particle-bound reactive oxygen species (ROS). Higher ws-Fe concentrations were observed in northern cities (Harbin, Beijing, and Xi'an) than in southern cities (Chengdu, Wuhan, and Guangzhou). Moreover, atmospheric ws-Fe concentrations in urban China were several folds higher than those in urban areas of the United States and several orders of magnitude higher than those in remote oceans, indicating that China is a key contributor to global atmospheric ws-Fe. The dominant form of ws-Fe was ws-Fe(III) in Beijing, whereas ws-Fe(II) was more abundant in the other five cities. The concentrations of ws-Fe and ws-Fe(II) concentrations increased with increasing PM2.5 levels in all the six cities, however, we did not observe any consistent pattern of ws-Fe(III) concentration. Biomass burning was a dominant source of ws-Fe in all cities except Beijing. A strong positive correlation was observed between particle-bound ROS content and ws-Fe; this finding is consistent with those of previous studies indicating that ws-Fe in PM2.5 notably influences atmospheric chemical processes and human health.

Incorporation and improvement of a heterogeneous chemistry mechanism in the atmospheric chemistry model GRAPES_Meso5.1/CUACE and its impacts on secondary inorganic aerosol and PM2.5 simulations in Middle-Eastern China.

Heterogeneous chemistry is considered one of the critical pathways of secondary inorganic aerosol (SIA) productions. In this study, a heterogeneous chemistry mechanism is incorporated into the atmospheric chemistry model GRAPES_Meso5.1/CUACE. Varying uptake coefficient schemes of SO2 and NO2 are compared and the equivalent ratio of inorganic aerosol (ER)-dependent scheme for SO2 and relative humidity (RH)/ER-dependent scheme for NO2 are used to form the improved heterogeneous chemistry. Focusing on a severe haze episode in Middle-Eastern China, the impacts of heterogeneous mechanism on SIA and PM2.5 composition are investigated based on the updated model. Study results show that the differences in RH or ER uptake coefficients result in obvious differences in sulfate and nitrate concentrations, especially during the severe pollution period, because the ER schemes restrict the excessive production of sulfate and nitrate under high RH effectively by including the self-limitation of heterogeneous reactions, which shows better performance in capturing the magnitude and temporal variations of surface SIA and PM2.5. Normalized mean bias of sulfate, nitrate, ammonium, and PM2.5 in megacity Beijing decreases from -27.0, -28.3, -58.2, and -26.3 to 1.0, -2.2, -47.2, and -16.5 %, respectively. And the fractions of sulfate, nitrate, ammonium, and organics during the polluted period change from 13.7, 19.3, 6.9, and 60.1 to 16.5, 23.0, 7.6, and 52.9 %, respectively, which is more consistent with the observation (16.0, 23.2, 14.1, and 46.7 %). SIA and PM2.5 simulations in another megacity Shanghai have the similar improvements. The modeled SIA by heterogeneous processes contributes 11.7 % of total PM2.5 in Beijing and 22.5 % in Shanghai. That is 13.5 % in the Chinese megalopolis Beijing-Tianjin-Hebei and 19.8 % in Yangtze-River-Delta, indicating a considerable contribution of heterogeneous pathways to haze pollution. This work indicates the importance of detailed and reasonable heterogeneous schemes for better SIA and haze/fog prediction in the atmospheric chemistry model.

Multi-Year Variation of Ozone and Particulate Matter in Northeast China Based on the Tracking Air Pollution in China (TAP) Data.

With the rapid development of economy and urbanization acceleration, ozone (O3) pollution has become the main factor of urban air pollution in China after particulate matter. In this study, 90th percentile of maximum daily average (MDA) 8 h O3 (O3-8h-90per) and PM2.5 data from the Tracking Air Pollution in China (TAP) dataset were used to determine the mean annual, seasonal, monthly, and interannual distribution of O3-8h-90per and PM2.5 concentrations in Northeast China (NEC). The O3-8h-90per concentration was highest in Liaoning (>100 µg/m3), whereas the highest PM2.5 concentration was observed mainly in urban areas of central Liaoning and the Harbin−Changchun urban agglomeration (approximately 60 µg/m3). The O3-8h-90per concentrations were highest in spring and summer due to more intense solar radiation. On the contrary, the PM2.5 concentration increased considerably in winter influenced by anthropogenic activities. In May and June, the highest monthly mean O3-8h-90per concentrations were observed in central and western Liaoning, about 170−180 µg/m3, while the PM2.5 concentrations were the highest in January, February, and December, approximately 100 µg/m3. The annual mean O3-8h-90per concentration in NEC showed an increasing trend, while the PM2.5 concentration exhibited an annual decline. By 2020, the annual mean O3-8h-90per concentration in southern Liaoning had increased considerably, reaching 120−130 µg/m3. From the perspective of city levels, PM2.5 and O3-8h-90per also showed an opposite variation trend in the 35 cities of NEC. The reduced tropospheric NO2 column is consistent with the decreasing trend of the interannual PM2.5, while the increased surface temperature could be the main meteorological factor affecting the O3-8h-90per concentration in NEC. The results of this study enable a comprehensive understanding of the regional and climatological O3-8h-90per and PM2.5 distribution at distinct spatial and temporal scales in NEC.

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.

Extensive characterization of aerosol optical properties and chemical component concentrations: Application of the GRASP/Component approach to long-term AERONET measurements.

A recently developed GRASP/Component approach (GRASP: Generalized Retrieval of Atmosphere and Surface Properties) was applied to AERONET (Aeronet Robotic Network) sun photometer measurements in this study. Unlike traditional aerosol component retrieval, this approach allows the inference of some information about aerosol composition directly from measured radiance, rather than indirectly through the inversion of optical parameters, and has been integrated into the GRASP algorithm. The newly developed GRASP/Component approach was applied to 13 AERONET sites for different aerosol types under the assumption of aerosol internal mixing rules to analyze the characteristics of aerosol components and their distribution patterns. The results indicate that the retrievals can characterize well the spatial and temporal variability of the component concentration for different aerosol types. A reasonable agreement between GRASP BC retrievals and MERRA-2 BC products is found for all different aerosol types. In addition, the relationships between aerosol component content and aerosol optical parameters such as aerosol optical depth (AOD), fine-mode fraction (FMF), absorption Ångström exponent (AAE), scattering Ångström exponent (SAE), and single scattering albedo (SSA) are also analyzed for indirect verifying the reliability of the component retrieval. It was demonstrated the GRASP/Component optical retrievals are in good agreement with AERONET standard products [e.g., correlation coefficient (R) of 0.93-1.0 for AOD, fine-mode AOD (AODF), coarse-mode AOD (AODC) and Ångström exponent (AE); R = ~ 0.8 for absorption AOD (AAOD) and SSA; RMSE (root mean square error) < 0.03 for AOD, AODF, AODC, AAOD and SSA]. Thus, it is demonstrated the GRASP/Component approach can provide aerosol optical products with comparable accuracy as the AERONET standard products from the ground-based sun photometer measurements as well as some additional important inside on aerosol composition.