Advances in sunphotometer-measured aerosol optical properties and related topics in China: Impetus and perspectives.

Aerosol is a critical trace component of the atmosphere. Many processes in the Earth's climate system are intimately related to aerosols via their direct and indirect radiative effects. Aerosol effects are not limited to these climatic aspects, however. They are also closely related to human health, photosynthesis, new energy, etc., which makes aerosol a central focus in many research fields. A fundamental requirement for improving our understanding of the diverse aerosol effects is to accumulate high-quality aerosol data by various measurement techniques. Sunphotometer remote sensing is one of the techniques that has been playing an increasingly important role in characterizing aerosols across the world. Much progress has been made on this aspect in China during the past decade, which is the work reviewed in this paper. Three sunphotometer networks have been established to provide high-quality observations of long-term aerosol optical properties across the country. Using this valuable dataset, our understanding of spatiotemporal variability and long-term trends of aerosol optical properties has been much improved. The radiative effects of aerosols both at the bottom and at the top of the atmosphere are comprehensively assessed. Substantial warming of the atmosphere by aerosol absorption is revealed. The long-range transport of dust from the Taklimakan Desert in Northwest China and anthropogenic aerosols from South Asia to the Tibetan Plateau is characterized based on ground-based and satellite remote sensing as well as model simulations. Effective methods to estimate chemical compositions from sunphotometer aerosol products are developed. Dozens of satellite and model aerosol products are validated, shedding new light on how to improve these products. These advances improve our understanding of the critical role played by aerosols in both the climate and environment. Finally, a perspective on future research is presented.

First in situ UV profile across the UTLS accompanied by ozone measurement over the Tibetan Plateau.

Ultraviolet radiation (UV) and ozone can greatly affect human health and the Earth's ecological environment. By deploying a UV radiometer aboard a stratospheric balloon released at Qaidam (QDM) during the Asian summer monsoon (ASM) period in 2019, we provided in situ measurement of the UV profiles from the surface to the upper troposphere and lower stratosphere over the Tibetan Plateau (TP), China, for the first time. Based on two in situ UV profiles accompanied by four ozonesonde measurements, this study exhibited detailed variations of downwelling UV and vertical ozone distributions over the TP during the ASM period. The UV differences between the surface and stratospheric balloon flight altitudes were 16.7, 15.8, 12.6 and 18.0 Wm-2 during the four ozonesonde launches. Due to the diurnal variations in photochemical production and the stratosphere-troposphere exchange, the integrated ozone columns below 30 km ranged from 184.4 to 221.6 DU from four ozonesonde measurements. A positive correlation between UV attenuation and ozone column was exhibited under low cloud cover and clear sky conditions. The results of this study are expected to improve our understanding of UV and ozone properties, as well as their potential effects on terrestrial ecosystems and living environments over this significant plateau.

Spatial and temporal distribution of the cloud optical depth over China based on MODIS satellite data during 2003-2016.

The cloud optical depth (COD) is one of the important parameters used to characterize atmospheric clouds. We analyzed the seasonal variations in the COD over East Asia in 2011 using cloud mode data from the AERONET (Aerosol Robotic Network) ground-based observational network. The applicability of the MODIS (Moderate Resolution Imaging Spectroradiometer) COD product was verified and compared with the AERONET cloud mode dataset. There was a good correlation between the AERONET and the MODIS. The spatial and temporal distribution and trends in the COD over China were then analyzed using MODIS satellite data from 2003 to 2016. The seasonal changes in the AERONET data and the time sequence variation of the satellite data suggest that the seasonal variations in the COD are significant. The result shows that the COD first decreases and then increases with the season in northern China, and reaches the maximum in summer and minimum in winter. However, the spatial distribution change is just the opposite in southern China. The spatial variation trend shows the COD in China decreases first with time and gradually increases after 2014. And the trend of COD in the western and central China is consistent with that in China. While the trend of COD shows a continuously increasing over time in northeast China and the Pearl River Delta.

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.

The feedback effects of aerosols from different sources on the urban boundary layer in Beijing China.

The interaction of aerosols and the planetary boundary layer (PBL) plays an important role in deteriorating urban air quality. Aerosols from different sources may have different effects on regulating PBL structures owing to their distinctive dominant compositions and vertical distributions. To characterize the complex feedback of aerosols on PBL over the Beijing megacity, multiple approaches, including in situ observations in the autumn and winter of 2016-2019, backward trajectory clusters, and large-eddy simulations, were adopted. The results revealed notable distinctions in aerosol properties, vertical distributions and thermal stratifications among three types of air masses from the West Siberian Plain (Type-1), Central Siberian Plateau (Type-2) and Mongolian Plateau (Type-3). Low loadings of 0.28 ± 0.26 and 0.15 ± 0.08 of aerosol optical depth (AOD) appeared in the Type-1 and Type-2, accompanied by cool and less stable stratification, with a large part (80%) of aerosols concentrated below 1500 m. For Type-3, the AOD and single scattering albedo (SSA) were as high as 0.75 ± 0.54 and 0.91 ± 0.05, demonstrating severe pollution levels of abundant scattering aerosols. Eighty percent of the aerosols were constrained within a lower height of 1150 m owing to the warmer and more stable environment. Large-eddy simulations revealed that aerosols consistently suppressed the daytime convective boundary layer regardless of their origins, with the PBL height (PBLH) decreasing from 1120 m (Type-1), 1160 m (Type-2) and 820 m (Type-3) in the ideal clean scenarios to 980 m, 1100 m and 600 m, respectively, under polluted conditions. Therefore, the promotion of absorbing aerosols below the residual layer on PBL could be greatly hindered by the suppression effects generated by both absorbing aerosols in the upper temperature inversion layer and scattering aerosols. Moreover, the results indicated the possible complexities of aerosol-PBL interactions under future emission-reduction scenarios and in other urban regions.

An examination of boundary layer structure under the influence of the gap winds in Urumqi, China, during air pollution episode in winter.

Tethered-sonde measurements of atmospheric profiles were performed at Urumuqi, capital of the Xinjiang Uyghur Autonomous Region of China, from 29 December 2008 to 14 January 2009. The data were used to examine the boundary layer structure during this severe air pollution period. Diurnal evolution of local wind flow near Urumqi was simulated using the fifth-generation Pennsylvania State University-National Center for Atmospheric Research (NCAR) Mesoscale Model (MM5). Measurements from operational radiosonde data showed that a southeasterly elevated low-level jet often intruded upon Urumqi through the middle Tianshan Mountain pass to the south of the city. The tethered-sonde measurements showed that calm and northwesterly winds prevailed near the surface in Urumqi, whereas the southeasterly winds of relatively higher speed were dominant above approximately 400 m. Both temperature inversion and humidity inversion frequently occured during day and nighttime. Temperature inversion intensity could sharply rise as the stronger elevated southeasterly gale (ESEG) happened. Model simulations showed that the winds near the surface around Urumqi remained calm during nighttime and developed toward the mountains during daytime. As cool airflow in the basin confronted the southeasterly winds from the pass in the lower layer, they formed a convergence line around Urumqi city, which was not favor for dilution of air pollutants.

Model analysis of vertical exchange of boundary layer ozone and its impact on surface air quality over the North China Plain.

In addition to photochemical production and horizontal regional transport, surface O3 concentration can also likely be affected by vertical transport, which is not well known so far. The process analysis was conducted by using the Regional Atmospheric Modeling System Community Multiscale Air Quality (RAMS-CMAQ) model to investigate photochemical production and the vertical transport mechanism of boundary-layer O3 during a typical O3 pollution episode in the North China Plain (NCP), and further quantify the contribution of vertical transport to surface O3. The diurnal variations of vertical budgets of O3 and NO2 in the boundary layer at multiple sites showed that there were substantial differences in the vertical distribution of O3 production and transport between urban and suburban/rural areas. In urban areas, surface O3 is consumed by titration reaction to generate NO2, which is then transported to the upper boundary layer and produces O3 by photochemical reaction. With the development of the boundary layer, the upper-layer O3 stored in the residual layer at nighttime can be transported vertically to the surface as the turbulent diffusion intensifies the next morning. While in suburban and rural areas, the vertical transport is relatively weaker because the photochemical formation of O3 occurs in the whole boundary layer, although it decreases slightly with the altitude. Model simulation showed that 20.6-27.9% of urban surface O3 changes in the morning (09:00-10:00 LST) was attributable to the downward transport from the residual layer, while it is 15.0-22.1% at suburban site. The vertical transport from above the boundary layer contributed 24.0-63.6% to daytime urban surface O3 changes, which was weak in suburban areas. Differences and similarities in O3 formation and transport mechanism in urban and suburban regions revealed here highlight the importance of earlier control and regional collaboration.

Emission, transport, deposition, chemical and radiative impacts of mineral dust during severe dust storm periods in March 2021 over East Asia.

A Regional Air Quality Model System (named RAQMS) coupled with a developed dust model driven by WRF was applied to synthetically investigate the emission, transport, deposition, budget, and chemical and radiative effects of mineral dust during the severe dust storm periods of 10-31 March 2021. Model results were validated against a variety of ground, vertical and satellite observations, which demonstrated a generally good model ability in reproducing meteorological variables, particulate matter and compositions, and aerosol optical properties. The first dust storm (DS1), which was the severest one since 2010 was originated from the Gobi Desert in southern Mongolia on 14 March, with the dust emission flux reaching 2785 µg m-2 s-1 and the maximum dust concentration exceeding 18,000 µg m-3 in the dust deflation region. This dust storm resulted in remarkably high hourly PM10 observations up to 7506 µg m-3, 1887 µg m-3, and 2704 µg m-3 in Beijing, Tianjin, and Shijiazhuang on 15 March, respectively, and led to a maximum decrease in surface shortwave radiation up to 313.4 W m-2 (72 %) in Beijing. The second dust storm (DS2) broke out in the deserts of eastern Mongolia, with lower dust emission than the first one. The extinction of shortwave radiation by dust aerosols led to a reduction in photolysis rate and consequently decreases in O3 and secondary aerosol concentrations over the North China Plain (NCP), whereas total sulfate and nitrate concentrations consistently increased due to heterogeneous reactions on dust surfaces over the middle reaches of the Yellow River and the NCP region during DS1. Sulfate and nitrate formation through heterogeneous reactions were enhanced in the dust backflow on 16-17 March by approximately 18 % and 24 % on average in the NCP. Heterogeneous reactions and photolysis rate reduction by mineral dust jointly led to average changes in sulfate, nitrate, ammonium, and secondary organic aerosol (SOA) concentrations by 13.0 %, 13.5 %, -12.3 %, and -4.4 %, respectively, in the NCP region during DS1, larger than the changes in the Yangtze River Delta (YRD). The maximum dry deposition settled in the 7-11 µm size range in downwind land and ocean areas, while wet deposition peaked in the 4.7-7 µm size range in the entire domain. Wet deposition was approximately twice the dry deposition over mainland China except for dust source regions. During 10-31 March, the total dust emission, dry and wet depositions were estimated to be 31.4 Tg, 13.78 Tg and 4.75 Tg, respectively, with remaining 12.87 Tg of dust aerosols (41 % of the dust emission) suspending in the atmosphere or transporting to other continents and oceans.

The influence of aerosols on the NO2 photolysis rate in a suburban site in North China.

The photolysis of NO2 is an important driving force of tropospheric ozone. The intensity of this photolysis reaction affects atmospheric oxidation and photochemical pollution process. Photolysis rate of nitrogen dioxide (JNO2) is affected by aerosols, temperature, solar zenith angle (SZA), clouds, and so on. Among them, aerosol is an important influencing factor because of its complicated and irregular change; aerosol quantitative effect on JNO2 is constructive for the coordinated control of O3 and particulate matter. In order to quantitatively assess the impact of aerosols on JNO2 in the long-term, the reconstructed JNO2 data in a suburban site in North China from 2005 to 2019 are used. We found that JNO2 and aerosol optical depth (AOD) presented logarithmic relations under different solar zenith angle (SZA) levels, the aerosol attenuation effect on JNO2 decreased as AOD increased. Two main influencing factors of JNO2, SZA, and AOD, were fitted into a quadratic polynomial to quantify the AOD effect on JNO2. The results showed that the average annual AOD effect on JNO2 in Xianghe from 2005 to 2019 was -28.6% compared to an aerosol free atmosphere; the seasonal mean AOD effect in spring, summer, autumn, and winter was -27.1% and -35.1%, -25.5% and -26.3%, respectively. During the study period, JNO2 increased with an average of 5 × 10-5 s-1 per year, while the annual average aerosol optical depth (AOD) was 0.80 ± 0.10, showing an overall downward trend. Annual mean AOD attenuation effect on JNO2 decreased over time; the decreases were larger in spring and summer, and smaller in autumn and winter.

Effect of source variation on the size and mixing state of black carbon aerosol in urban Beijing from 2013 to 2019: Implication on light absorption.

Black carbon (BC) is the most important aerosol light-absorbing component, and its effect on radiation forcing is determined by its microphysical properties. In this study, two microphysical parameters of refractory BC (rBC), namely, size distribution and mixing state, in urban Beijing from 2013 to 2019 were investigated to understand the effects of source changes over the past years. The mass equivalent diameter of rBC (Dc) exhibited bimodal lognormal distributions in all seasons, with the major modes accounting for most (>85%) of the rBC masses. The mass median diameter (MMD) was obviously larger in winter (209 nm) than in summer (167 nm) likely due to the contribution of more rBC with larger Dc from solid fuel combustion and enhanced coagulation of rBC in polluted winter. More rBC particles were thickly coated in winter, with the number fraction of thickly coated rBC (fcoatBC) ranging within 29%-48% compared with that of 12%-14% in summer. However, no evidential increase in BC light-absorption capability was observed in winter. This finding was likely related to the lower absorption efficiency of larger rBC in winter, which partly offset the coating-induced light enhancement. Two stage of decreases in MMD and fcoatBC were observed, accompanied with a persistent decrease in rBC loading, thereby reflecting the discrepant effects of source control measures on rBC loading and physical properties. The control measures in the earlier stage before 2016 was more efficient to reduce the rBC loading but slightly influenced the microphysical properties of rBC. As of 2016, the reduction in rBC concentration slowed down because of its low atmospheric loading. However, rBC showed a more obvious decrease in its core size and became less coated. The decrease in fcoatBC may have weakened the BC absorption and accelerated the decrease in light absorption resulting from the reduction in rBC loading.

Spectral absorption properties of organic carbon aerosol during a polluted winter in Beijing, China.

A fraction of organic carbon (OC) is found to exhibit the capability to absorb solar radiation. However, the absorption properties of OC remain poorly characterized partly due to uncertainties in determination methods. In this study, the absorption coefficient (bap) of OC (bap,OC) in Beijing during a polluted winter was estimated on the basis of the combined measurements of black carbon (BC) size distribution and total aerosol bap (bap,meas). The bare BC bap (bap,bareBC) calculated using Mie theory on the basis of measured size distribution exhibited weak wavelength dependence, with a mean absorption Ångström exponent (AAE) of 0.56 ± 0.04 within the 470-660 nm wavelength range, which was lower than the value of 1 commonly used for freshly emitted BC. The calculated bap,bareBC was compared with bap,meas at 950 nm to derive the coating thickness of BC, from which the calculation of coated BC bap (bap,coatBC) within 370-660 nm was based using the core-shell Mie model. Given the thick coatings, the AAE of coated BC, with a mean of 0.53 ± 0.12, was slightly lower than that of bare BC. Subsequently, bap,OC was obtained by subtracting bap,coatBC from bap,meas, accounting for 59.57 ± 4.82% of bap,meas at 370 nm on average. The average mass absorption efficiency of OC was estimated to be 1.48 ± 0.36 m2 g-1 at 370 nm. bap,OC significantly decreased as wavelength increased, deriving an AAE of OC with a mean of 2.72 ± 0.32 within the 370-660 nm range. The level of bap,OC estimated on the basis of a widely used attribution method assuming a constant BC AAE of 1 was ~60% lower than the currently presented value, probably underestimating OC radiative effect by a factor of >3. More accurate estimations of bap,OC based on more advanced measurements and suitable theory calculations are recommended to provide more reliable assessments of OC radiative effects.

Variation in black carbon concentration and aerosol optical properties in Beijing: Role of emission control and meteorological transport variability.

Black carbon (BC), which is a by-product with incomplete combustion of carbonaceous materials, can be used as an indicator of combustion emissions and is an important climate forcer. In this study, a spatial-temporal synthesis of BC aerosols and the affecting factors was conducted in urban Beijing. As observed, BC showed a spatial pattern with high concentration in south and low in north. BC concentration evidently decreased by approximately 61% between 2005 and 2017. From 2015 to 2017, the mass ratio of BC/PM2.5 dropped by 28%, which suggested a more efficient effect of control measures to BC than PM2.5. The BC/CO ratio dropped by 22%, which indicated the decreasing emission from fossil fuel sources. With regard to BC loading, the spectral dependence of absorption aerosol exhibited significant seasonal variations. High absorption Ångström exponent (α) was observed during heating season, which reflected the increasing contribution of brown carbon (BrC) to light absorption. Backward trajectory analysis showed that the levels of BC and PM2.5 were high in Cluster-South and Cluster-West. BrC absorption was high in Cluster-West, Cluster-Northwest and Cluster-Northeast, due to the biomass and coal burning for domestic heating and aging processes on a regional scale. The effects of emission control and transport variability on pollutant variation were estimated on the basis of the cluster analysis. Results indicated that the effect of emission reduction was the major reason for the decrease of BC from 2015 to 2017, which resulted in a 34% reduction of BC concentration. Meanwhile, transport variability caused a 15% reduction.

Aerosol optical properties and its type classification based on multiyear joint observation campaign in north China plain megalopolis.

Since haze and other air pollution are frequently seen in the North China Plain (NCP), detail information on aerosol optical and radiative properties and its type classification is demanded for the study of regional environmental pollution. Here, a multiyear ground-based synchronous sun photometer observation at seven sites on North China Plain megalopolis from 2013 to 2018 was conducted. First, the annual and seasonal variation of these characteristics as well as the intercomparsion were analyzed. Then the potential relationships between these properties with meteorological factors and the aerosol type classification were discussed. The results show: Particle volume exhibited a decreasing trend from the urban downtown to suburban and the rural region. The annual average aerosol optical depth at 440 nm (AOD440) varied from ∼0.43 to 0.86 over the NCP. Annual average single-scattering albedo at 440 nm (SSA440) varied from ∼0.89 to 0.93, indicating a moderate to slight absorption capacity. Average absorption aerosol optical depth at 440 nm (AAOD440) varied from ∼0.07 to 0.10. The absorption Ångström exponent (AAE) (∼0.89-1.40) indicated the multi-types of absorptive matters originated form nature and anthropogenic emission. The discussion of aerosol composition showed a smaller particle size of aerosol from biomass burning and/or fossil foil consumption with enhanced aerosol scattering and enlarged light extinction. Aerosol classification indicated a large percentage of mixed absorbing aerosol (∼20%-49%), which showed increasing trend between relative humidity (RH) with aerosol scattering and dust was an important environmental pollutant compared to southern China.

Analysis of water vapor effects on aerosol properties and direct radiative forcing in China.

The effects of column water vapor (CWV) on aerosol optical properties, radiative effects and classification are studied by using aerosol and CWV data from eight Aerosol Robotic Network (AERONET) sites in China: Beijing, XiangHe, Shouxian, Taihu, Hong_Kong, Zhongshan_Univ, SACOL, and Mt_WLG, which represents 5 distinct aerosol climatologies in China. Contrast in correlations between aerosol optical depth (AOD) and CWV is found. High correlation coefficient (R) ranging from 0.63-0.94 is observed at Beijing and XiangHe (North China Plain), SACOL (Northwest China) and Mt_WLG (the Tibetan Plateau). R values at stations in the Middle-East China (Shouxian and Taihu) are within 0.32-0.45. AOD shows poor correlation to CWV in Southeast China (R at Hong_Kong and Zhongshan_Univ of 0.15 and 0.27). At most sites, the asymmetry (ASYM) of fine-mode aerosol increases with CWV with R larger than ~0.4. Aerosol direct radiative forcing efficiency (ADRFE) at the bottom of the atmosphere (BOA) is affected by CWV, with R >~0.5 over the north and Middle-East China sites. The statistic results show that an increase of CWV by 0.1 cm could result in enhancements of ADREF at the BOA by about 1.1-2.8 W m-2 at all the sites except Mt_WLG. The aerosol classification shows that the mix-small aerosol type is always dominated under the high CWV air. The clusters of back-trajectories with relative humidity (RH) from Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model indicate that the air mass with high RH is often from south and east directions. The influence of CWV on aerosol properties is mainly shown in the properties of fine mode aerosol, which needs to be considered in the study of aerosol radiative forcing and climate effects.

Long-term validation of MODIS C6 and C6.1 Dark Target aerosol products over China using CARSNET and AERONET.

This study provided a comprehensive evaluation of the Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 006 (C6) and 061 (C6.1) Dark Target (DT) 10 km aerosol optical depth (AOD) over China during 2002-2014. Considering that sparse Aerosol Robotic Network (AERONET) sites are available in China, 18 sites from China Aerosol Remote Sensing Network (CARSNET) were also used to conduct this validation. The results showed that C6.1 DT outperform C6 with 59.03% of the retrievals falling within the expected error (EE) compared to C6 (54.94%). Meanwhile, C6.1 DT achieved a reduced RMSE of 0.171, a higher R of 0.901 and a bias closer to 0 relative to C6 (RMSE: 0.185; R: 0.890). When the validation was conducted over different underlying surfaces, C6 DT overestimated AOD by 19.8%, with only 45.01% of the retrievals within the EE over urban sites, whereas C6.1 showed clear improvements, with 11.8% more data falling within the EE. Hardly any improvement was observed in C6.1 over forest, cropland, and grassland sites. The C6.1 DT exhibited more significant improvements over Beijing area and northern China than southern China. The highest retrieval accuracy of 61.05% among the four Beijing sites was achieved at Beijing_CARSNET, but the improvements were lower than other Beijing sites. The extent of the improvements was positively correlated with the percentage of urban pixels over the sites in Beijing and northern China in terms of the retrieval accuracy. Moreover, C6.1 DT had a little effect on improvements over southern China and showed reduced collocation over coastal cities.

Characterization of vertical distribution and radiative forcing of ambient aerosol over the Yangtze River Delta during 2013-2015.

As the central part of eastern China, the Yangtze River Delta (YRD) region, with its rapid economic growth and industrial expansion, has experienced severe air quality issues. In this study, the monthly variation and interaction between aerosol direct radiative forcing (ADRF) and aerosol vertical structure during 2013-2015 over the YRD were investigated using ground-based observations from a Micro Pulse Lidar (MPL) and a CE-318 sun-photometer. Combining satellite products from MODIS and CALIPSO, and reanalysis wind fields, an integrated discussion of a biomass burning episode in Hangzhou during August 2015 was conducted by applying analysis of optical properties, planetary boundary layer (PBL), spatial-temporal and vertical distributions, backward trajectories, Potential Source Contribution Function (PSCF), and Concentration Weighted Trajectory (CWT). The results reveal that a shallower PBL coincides with higher scattering extinction at low altitude, resulting in less heating to the atmosphere and radiative forcing to the surface, which in turn further depresses the PBL. In months with a deeper PBL, the extinction coefficient decreases rapidly with altitude, showing stronger atmospheric heating effects and ADRF to the surface, facilitating the turbulence and vertical diffusion of aerosol particles, which further reduces the extinction and raises the PBL. Because of the hygroscopic growth facilitated by high relative humidity, June stands out for its high scattering extinction coefficient and relatively low PBL, and the reduced ADRF at the surface and the enhanced cooling effect on near-surface layer in turn depresses the PBL. Absorptive aerosols transported from biomass burning events located in Zhejiang, Jiangxi, and Taiwan provinces at 1.5 km, result in high ADRF efficiency for atmospheric heating. And the enhanced heating effect on near-surface layer caused by absorptive particles facilitates PBL development in August over the YRD.

Five-year observation of aerosol optical properties and its radiative effects to planetary boundary layer during air pollution episodes in North China: Intercomparison of a plain site and a mountainous site in Beijing.

The aerosol microphysical, optical and radiative properties of the whole column and upper planetary boundary layer (PBL) were investigated during 2013 to 2018 based on long-term sun-photometer observations at a surface site (~106 m a.s.l.) and a mountainous site (~1225 m a.s.l.) in Beijing. Raman-Mie lidar data combined with radiosonde data were used to explore the aerosol radiative effects to PBL during dust and haze episodes. The results showed size distribution exhibited mostly bimodal pattern for the whole column and the upper PBL throughout the year, except in July for the upper PBL, when a trimodal distribution occurred due to the coagulation and hygroscopic growth of fine particles. The seasonal mean values of aerosol optical depth at 440 nm for the upper PBL were 0.31 ±â€¯0.34, 0.30 ±â€¯0.37, 0.17 ±â€¯0.30 and 0.14 ±â€¯0.09 in spring, summer, autumn and winter, respectively. The single-scattering albedo at 440 nm of the upper PBL varied oppositely to that of the whole column, with the monthly mean value between 0.91 and 0.96, indicating weakly to slightly strong absorptive ability at visible spectrum. The monthly mean direct aerosol radiative forcing at the Earth's surface and the top of the atmosphere varied from -40 ±â€¯7 to -105 ±â€¯25 and from -18 ±â€¯4 to -49 ±â€¯17 W m-2, respectively, and the maximum atmospheric heating was found in summer (~66 ±â€¯12 W m-2). From a radiative point of view, during dust episode, the presence of mineral dust heated the lower atmosphere, thus promoting vertical turbulence, causing more air pollutants being transported to the upper air by the increasing PBLH. In contrast, during haze episode, a large quantity of absorbing aerosols (such as black carbon) had a cooling effect on the surface and a heating effect on the upper atmosphere, which favored the stabilization of PBL and occurrence of inversion layer, contributing to the depression of the PBLH.

Synergy of AERONET and MODIS AOD products in the estimation of PM2.5 concentrations in Beijing.

Satellite aerosol optical depth (AOD) is widely used to estimate particulate matter with aerodynamic diameter ≤2.5 µm (PM2.5) mass concentrations. Polar orbiting satellite retrieval 1-2 times each day is frequently affected by cloud, snow cover or misclassification of heavy pollution. Novel methods are therefore required to improve AOD sampling. Sunphotometer provides much more AODs than satellite at a fixed point. Furthermore, much of the aerosol pollution is regional. Both factors indicate that sunphotometer has great potential for PM2.5 concentration estimation. The spatial representativeness of the Aerosol Robotic Network (AERONET) AOD at Beijing site is investigated by linear regression analysis of 13-year daily paired AODs at each grid from Moderate Resolution Imaging Spectroradiometer (MODIS) on Aqua and Beijing AERONET. The result suggests a good correlation for the whole Beijing Administrative region, with regional mean correlation coefficient exceeding 0.73. Pixel AODs are then estimated from AERONET AOD using linear equations, which are verified to have the same accuracy as that of MODIS AOD. Either AOD from MODIS retrieval or estimation from AERONET AOD in the absence of MODIS pixel AOD is finally used to predict PM2.5 concentration. Daily AOD sampling in average is enhanced by 59% in winter when MODIS AODs are very limited. More importantly, synergy of AERONET and MODIS AOD is able to improve the estimation of regional mean PM2.5 concentrations, which indicates this method would play a significant role in monitoring regional aerosol pollution.

Evaluation of aerosol optical depth and aerosol models from VIIRS retrieval algorithms over North China Plain.

The first Visible Infrared Imaging Radiometer Suite (VIIRS) was launched on Suomi National Polar-orbiting Partnership (S-NPP) satellite in late 2011. Similar to the Moderate resolution Imaging Spectroradiometer (MODIS), VIIRS observes top-of-atmosphere spectral reflectance and is potentially suitable for retrieval of the aerosol optical depth (AOD). The VIIRS Environmental Data Record data (VIIRS_EDR) is produced operationally by NOAA, and is based on the MODIS atmospheric correction algorithm. The "MODIS-like" VIIRS data (VIIRS_ML) are being produced experimentally at NASA, from a version of the "dark-target" algorithm that is applied to MODIS. In this study, the AOD and aerosol model types from these two VIIRS retrieval algorithms over the North China Plain (NCP) are evaluated using the ground-based CE318 Sunphotometer (CE318) measurements during 2 May 2012 - 31 March 2014 at three sites. These sites represent three different surface types: urban (Beijing), suburban (XiangHe) and rural (Xinglong). Firstly, we evaluate the retrieved spectral AOD. For the three sites, VIIRS_EDR AOD at 550 nm shows a positive mean bias (MB) of 0.04-0.06 and the correlation of 0.83-0.86, with the largest MB (0.10-0.15) observed in Beijing. In contrast, VIIRS_ML AOD at 550 nm has overall higher positive MB of 0.13-0.14 and a higher correlation (0.93-0.94) with CE318 AOD. Secondly, we evaluate the aerosol model types assumed by each algorithm, as well as the aerosol optical properties used in the AOD retrievals. The aerosol model used in VIIRS_EDR algorithm shows that dust and clean urban models were the dominant model types during the evaluation period. The overall accuracy rate of the aerosol model used in VIIRS_ML over NCP three sites (0.48) is higher than that of VIIRS_EDR (0.27). The differences in Single Scattering Albedo (SSA) at 670 nm between VIIRS_ML and CE318 are mostly less than 0.015, but high seasonal differences are found especially over the Xinglong site. The values of SSA from VIIRS_EDR are higher than that observed by CE318 over all sites and all assumed aerosol modes, with a positive bias of 0.02-0.04 for fine mode, 0.06-0.12 for coarse mode and 0.03-0.05 for bi-mode at 440nm. The overestimation of SSA but positive AOD MB of VIIRS_EDR indicate that other factors (e.g. surface reflectance characterization or cloud contamination) are important sources of error in the VIIRS_EDR algorithm, and their effects on aerosol retrievals may override the effects from non-ideality in these aerosol models.

Quantification of the impact of aerosol on broadband solar radiation in North China.

PM2.5 plays a key role in the solar radiation budget and air quality assessments, but observations and historical data are relatively rare for Beijing. Based on the synchronous monitoring of PM2.5 and broadband solar radiation (Rs), a logarithmic function was developed to describe the quantitative relationship between these parameters. This empirical parameterization was employed to calculate Rsn from PM2.5 with normalized mean bias (NMB) -0.09 and calculate PM2.5 concentration from Rsn with NMB -0.12. Our results indicate that this parameterization provides an efficient and straightforward method for estimating PM2.5 from Rs or Rs from PM2.5.