Black carbon (BC) significantly influences climate, air quality, and public health, and long-term observations are essential for understanding its adverse effects. While previous studies have primarily focused on spatiotemporal variations, deeper insights from such datasets remain uncovered. Using 13 years (2008–2020) of continuous measurements of equivalent black carbon (eBC) in China, this study reported the spatial-temporal variations of eBC and its sources, including solid fuel (eBCsf) and liquid fuel combustion (eBClf). The results showed that eBC and its sources exhibited higher concentrations in eastern and northern China compared to western and southern China. Seasonal variations of eBC and eBCsf generally showed lower values during summer and higher values during winter at most stations. Long-term trends indicated that eBC and eBClf decreased most rapidly at urban stations, while eBCsf declined faster at rural stations. Comparisons of eBC concentrations and trends between this study and global observations revealed higher eBC levels but lower reduction rates in China. These long-term observations showed that the model simulations performed well in simulating spatial distribution but poorly in capturing inter-annual variations. The weather-normalized eBC concentrations showed potential for adjusting emission estimates. The normalized results also suggested that emission control was the dominant driver of the BC reduction. This decrease was primarily driven by reductions from solid fuel combustion at rural and background stations. This study provides insights for reducing uncertainties in black carbon emission inventories and improving model performance in simulating surface concentrations.
Particulate organic nitrates (pON) significantly contribute to the mass of organic aerosol and influence the nitrogen oxides cycle in the atmosphere, but their evolution and lifetime remain uncertain. This study performed simultaneous measurements on the anthropogenically affected surface site and the mountain site on top of the polluted planetary boundary layer (PBL). After aging in the PBL, organic nitrate was converted from primary sources (decreased from 8.7% to 4.3%) to secondary sources (increased from 6.3% to 36.1%), spanning from the surface to the mountain. The evaporation of more volatile inorganic nitrate and the production of secondary organic nitrate during aging in the PBL contributed to the enhanced pON fraction over the top of PBL. The contribution of light absorption by brown carbon increased by 57% at the top of PBL compared to the surface, consistent with the higher fraction of nitrogenous organic aerosols over the mountain. The results provide field evidence that the nitrogenous organic aerosols (OA) may be preserved by adding into secondary OA and significantly contribute to the enhanced importance of brown carbon after aging during vertical transport in the PBL.
The vertical structure of meteorological elements, black carbon (BC), and aerosols were in situ characterized by the King Air 350 aircraft measurements over the northeast of China during an East Asian dust storm event from April 10 to 13, 2023. The main causes of this dust storm event were the strong winds generated by the Mongolian cyclone, the cold front on the ground provided dynamic conditions, and the unstable atmospheric state provided thermal conditions and less precipitation in the dust source areas led to exposed the ground surface. The number concentrations of BC and aerosol had significant vertical distribution. The number concentration of aerosol in the dust storm (DS) layer increased rapidly with height, while the number and mass concentrations of BC were higher and varied slightly with height. The BC core mass median diameters (MMD) first increased with height, reaching a maximum value of 0.24μm at 3000m; and it rapidly decreased to 0.18μm at 3200m and then varied slightly with height above 3200m. BC's bulk relative coating thickness (coated diameter divided by uncoated core diameter Dp/Dc) first decreased with height, reaching a minimum value of 1.16 at 3000m, then increased with height, reaching a maximum of 1.38 (4250m). A wind shear layer (7.9 m·s−1 at 1850 m) with a sudden drop in temperature (the cooling rate can reach 7.4 °C·(100 m)−1) at 1900 m hinders the transportation of dust particles to the ground, allowing the dust particles to be transported at long-term distances. There were two stratifications in the dust storm layer: DS1 (1700–3000 m, the vertical wind speed was downward, the horizontal wind speed was small) and DS2 (3000–4500 m, the vertical wind speed was upward, the horizontal wind speed was large). The distinct atmospheric flow field conditions between DS1 and DS2 led to different BC and aerosol pollution characteristics. In DS2, the number concentrations of BC and aerosol were higher, the aging ratio of BC particles was higher, and the size of the core particle of BC was smaller. The concentrations of BC, aerosol, Dp/Dc, and MMD in DS2 were 1.1, 59.0, 1.02, and 0.84 times higher than those in DS1, respectively. Dust particles transported over long distances were primarily small. The number concentrations of aerosols at 0.1–0.12 μm and 0.1–0.24 μm were higher in DS1 and DS2, respectively. Still, the number concentration of aerosol at 0.12–0.28 μm in DS1 was lower than in the planetary boundary layer (PBL) and residual layer (RL).
The microphysical properties associated with ice production importantly determine precipitation rates. In this study, the microphysical properties of stratiform clouds with embedded convection during an extratropical cyclone over northern China were characterized in situ. Stages of clouds, including young cells rich in liquid water and developing and mature stages with high number concentrations of ice particles (NIce), were investigated. NIce could reach 300 L-1 in the mature stage, approximately 2 orders of magnitude higher than the primary NIce. The secondary ice production (SIP) rate was 0.005-1.8 L-1 s-1, which was derived from the measured NIce. The SIP rate could be produced using a simplified collision-coalescence model by considering the collection of large droplets by graupel. The collection efficiency between the graupel and the droplet was found to increase when the size of the droplet approached that of the graupel, which may improve the agreement between the measurements and the model. Importantly, the overall NIce was found to be highly related to the distance to the cloud top (DCT). The level with a larger DCT had more rimed graupel falling from the upper levels, which promoted coalescence processes between the graupel and the droplets, producing a greater fraction of smaller ice. This seeder-feeder process extended the avalanche SIP process at lower temperatures to -14 degrees C, beyond the temperature region of the Hallett-Mossop process. The results illustrate the microphysical properties of clouds with convective cells at different stages, which will improve the understanding of the key processes in controlling the cloud glaciation and precipitation processes.
Abstract. The microphysical properties associated with the ice production importantly determine the precipitation rate of clouds. In this study, the microphysical properties including the size distribution and particle morphology of water and ice for stratocumulus during an extratropical cyclone over the northern China were in-situ characterized. Stages of cloud were investigated including young cells rich of liquid water, developing and mature stages with high number concentration of ice particles (Nice). The Nice could reach 300 L-1 at the mature stage, about two orders of magnitudes higher than the primary ice number concentration calculated from ice nucleation. This high Nice occurred at about −5 to −12 °C, spanning the temperature region of Hallett-Mossop process and possible other mechanisms for the secondary ice production (SIP). The Nice was positively associated with the number concentrations of large graupel with diameter (d) > 250 μm and large supercooled droplet (d > 50 μm). The SIP rate was 0.005-1.8 L-1s-1 derived from the measured Nice with known ice growth rate between two sizes. The SIP rate could be produced by a simplified collision-coalescence model within an uncertainty factor of 5, by considering the collection of large droplets by graupel. The collection efficiency between was found to increase when the size of droplet was closer to graupel which may improve the agreement between measurement and model. Importantly, the overall Nice was found to be highly related to the distance to cloud-top (DCT). The level with larger DCT had more abundant rimmed graupels falling from the above level, which promoted the coalescence processes between graupels and droplets, producing a higher fraction of smaller ice through SIP. This seeder-feeder process extended the avalanche SIP at lower temperature up to −14 °C beyond the temperature region of Hallett-Mossop process. The results illustrated the microphysical properties of clouds with convective cells under different stages, which will improve the understanding of the key processes in controlling the cloud glaciation and precipitation process.
The microphysical and dynamic evolution characteristics of two convections (labeled A and B) were analyzed using polarimetric radars during the same weather conditions under the influence of ground-based rockets and artilleries containing silver iodide (AgI). The ice and liquid water content (IWC and LWC, respectively), hydrometeor classification and three-dimensional wind structure were retrieved to analyze the convection evolution. The results indicate that the convective evolution trends after AgI seeding are related to the preoperation dynamic and microphysical structure. The ice processes of convection A are more active before operation, with a high echo center of gravity, larger IWC and LWC, and a predominance of graupel above the freezing level. The center of gravity of the convection gradually decreases, and the cloud collapses and gradually dissipates during AgI seeding. Convection B has more active liquid processes, with a stronger updraft but lower IWC and LWC. During AgI seeding, ice processes of the convection have a tendency to be enhanced, with a higher echo center of gravity and increases in IWC, and LWC below the freezing level. During significant wind shear, the path of convection may tend to align with the background guided flow at different levels, depending on the different intensities of convection influenced by AgI seeding. The convection intensity and its matching with vertical wind shear should be considered when artificially seeding convection.
The microphysical attributes of black carbon (BC) can determine its absorption and hygroscopic properties. However, long-term information is difficult to obtain from the field. In this study, the BC properties including mass concentration, the coating volume ratio (VR) relative to the refractory BC (rBC), the rBC diameter and the fraction of cloud condensation nuclei (CCN), are derived from a number of field experiments using a random forest model. This model effectively derives the long-term BC microphysical properties in the Beijing region from 2013 to 2020 using continuous measurements of particulate matter, gas, BC mass concentration and meteorological parameters. The results reveal notably higher BC coatings (mean VR = 7.2) and a greater fraction of CCN-like BC (51%) in the winter compared to other seasons. Following the implementation of national air pollution control measures in 2017, BC mass exhibited a substantial reduction of 60% (29%) in the winter (summer), and VR decreased by 45% (24%). Apart from the influence of meteorological variations, these can be attributed to the declined primary emissions and the gas precursors which are associated with secondary formation of BC coatings. The reduction of both BC mass loading and coatings leads to its solar absorption decreasing by 50%, and the fraction of CCN-like BC (likely in clouds) decreasing by 23%. Environmental regulation will therefore continue to reduce both direct and indirect radiative impacts of BC in this region.
In this study, joint observations of the airborne Ka-band precipitation radar (KPR) and Himawari-8 were used to investigate the underlying links among cloud macro and microphysical parameters such as cloud top height (CTH), effective particle radius (Re), and cloud top temperature (CTT). Our results indicate that, compared to CTH from the Himawari-8 products (CTH Himawari), CTH detected by KPR (CTHKPR) is mostly lower, with a difference (Delta H) ranging from 0.5 km to 3 km. Statistics of 11 flight observations over North China Plain reveal a non-monotonous dependence of Delta H on Re, while Delta H is well correlated with CTT. In addition, larger particles as observed by Himawari-8 around cloud tops are characterized by more significant size growth than smaller ones, which may be attributed to more efficient aggregation. Two events with small and medium-to-large Re are analyzed, respectively.
The cloud condensation nuclei (CCN) activity of black carbon (BC) particles importantly determines their impacts on cloud microphysics and atmospheric lifetime. This process is crucially influenced by the number of hygroscopic coating materials that BC acquire during the ageing process. It remains a challenge for ambient measurements to capture this process and link this with CCN activity of BC. Here, we directly measured the droplet activation diameter (D50) and activation fraction of BC-containing (BCc) particles (Fact,BC) in suburban Beijing using coupled measurements of size-resolved number concentrations of CCN at configured water supersaturation (SS) and BCc particles. The number concentration of BCc particles was found to peak at diameter 180–210 nm after acquiring coatings, larger than that for all particles (50–150 nm). Consequently, the initially smaller BC particles become enlarged and more hygroscopic, thereby exhibiting CCN activities than other particles. The Fact,BC increased from 42 % to 69 % in number and from 67 % to 85 % in mass as SS increased from 0.1 % to 0.2 % but tended to reach a plateau when SS > 0.2 %. Notably, Fact,BC and D50 linearly correlated with equivalent photochemical age, at a rate of +2 % h−1 and −3 nm h−1, respectively. The results suggest BCc particles from anthropogenic sources can readily serve as CCN at a relatively low SS, and more than half of the BC population can be activated within a few hours, indicating that the surface-sourced BC can efficiently incorporate into clouds and potentially exert important indirect radiative impacts.
The light-absorbing organic aerosol (OA), known as brown carbon (BrC), has important radiative impacts; however, its sources and evolution after emission remain to be elucidated. In this study, the light absorption at multiple wavelengths, mass spectra of OA and microphysical properties of black carbon (BC) were characterized at a typical suburban environment in Beijing. The absorption of BC is constrained by its size distribution and mixing state, and the BrC absorption is obtained by subtracting the BC absorption from the total aerosol absorption. Aerosol absorption was further apportioned to BC, primary BrC and secondary BrC by applying the least correlation between secondary BrC and BC. The multilinear regression analysis on the factorized OA mass spectra indicated that the OA from traffic and biomass burning emission contributed to primary BrC. Importantly, the moderately oxygenated OA (O / C = 0.62) was revealed to highly correlate with secondary BrC. These OA had higher nitrogen content, in line with the nitrogen-containing functional groups detected by the Fourier transform infrared spectrometer. The photochemical processes were found to reduce the mass absorption cross section (MAC) of primary OA, reducing its contribution to total absorption by 20 %, at the same time increasing MAC for secondary OA, which showed a 30 % enhancement in contribution to total absorbance, implying the concurrent whitening and darkening of BrC. This provides field evidence that the photochemically produced secondary nitrogen-containing OA can considerably compensate for some bleaching effect on the primary BrC, hereby causing radiative impacts.
The uncertainty of the climatic effect of Black carbon (BC) remains large. One critical uncertainty source that needs to be captured is BC aging. Here we use the Community Atmosphere Model version 6 (CAM6) configured with the four‐mode version of the Modal Aerosol Module (MAM4) to evaluate the modeled BC aging process with recent laboratory and in‐situ measurements over China. As revealed by the comparison of BC aging timescale and number fraction of aged BC against recent measurements, the modeled condensation aging timescale is estimated to be about 0.8 hr (17%) faster than the chamber measurement, and the diurnal variations of modeled BC aging degree are typically higher than observations mainly due to the fast increase in modeled BC aging degree during daytime. Further analysis shows that the condensation aging dominates (>70%) BC aging across China. More specifically, the condensation of secondary organic aerosol (SOA) vapor contributes most to BC aging over China. Slowing down BC aging increases the modeled surface BC concentration over remote Western China and BC burden, but hardly changes surface BC concentration over Eastern China. Our results suggest that BC aging representation in the MAM4 needs to be further improved toward slowing down the BC aging rate, especially the condensation aging by SOA, to improve the BC simulation over remote areas and its impact on BC transport in MAM4.
Based on in-situ measurement of black carbon (BC) and carbon monoxide (CO), the characteristics of BC emissions and wet scavenging were comprehensively investigated in Nanning, South China. The average annual BC concentration was 1.02 ± 0.53 μg m-3 with higher pollution levels during winter. In winter, a higher net BC/CO (ΔBC/ΔCO) ratio of 3.3 ± 0.3 ng m-3 ppb-1 along with an increased absorption Ångström exponent (AAE) and BC mass from biomass burning (BCbb), indicated a significant contribution of biomass burning to BC emissions. However, emissions from the traffic sector consistently exerted a dominant influence throughout the year. Cluster analysis of backward trajectories identified three types of air masses with distinct origins. Cluster #1 originated from Guangxi province and its vicinity, intermittently influencing the sampling site throughout the year with varying effects between winter and summer. This air mass brought in clean sea breeze in summer whereas transported a higher proportion of BCbb to the site during wintertime due to local open biomass burning. Cluster #3 primarily arrived in autumn and winter (October-December) from polluted central China, resulting in substantially high BC mass at the site. Cluster #2 coincided with the period (January-March) when extensive surface open biomass burning events occurred in Southeast Asia (SEA) regions. These BC aerosols in cluster#2 initially rose to higher altitudes above SEA before being regionally transported, but were significantly scavenged by clouds and precipitation during vertical uplift. The remaining BC exhibited a notably lower BC loss rate on relative humidity (RH) of -0.01 ng m-3 ppb-1 %-1 compared to cluster #1 (-0.03) and cluster #3 (-0.06), corresponding to an average BC transport efficiency of 0.85, 0.73, and 0.53, respectively. Nonetheless, air masses in cluster #2 could still transport considerably high BC mass to Nanning due to dry conditions and less wet scavenging along trajectory pathways. These findings provide valuable insights for policymakers and government officials in regulating and mitigating BC pollution in South China.
To better understand the influence of aerosols on micro-properties of clouds and to facilitate weather modification experiments including the analysis of various materials' seeding effect on clouds and precipitation, Beijing Weather Modification Center has taken a decisive step forward by constructing an advanced facility known as Beijing aerosol and cloud interaction chamber (BACIC) in suburban Pinggu district. Boasting an impressive volume of 70 m3, BACIC is not only the largest of its kind in operation in China, but also a testament to the scale of the country's commitment to this sphere of atmospheric science. The enormity of the chamber's capacity facilitates the performance of a broad spectrum of investigations, thus enhancing the comprehensiveness and reliability of the results obtained.Inside BACIC, advanced instrumentation allows for the meticulous measurement and control of temperature, relative humidity, and background aerosol concentration. During 2019-2021, the chamber's capabilities extend further, as demonstrated by successful tests of its ability to create liquid and mixed-phase clouds. These attributes, combined with its capacity to control the cloud droplet size distribution as proved by comparative experiments involving changes in expansion rate and aerosol number concentration, solidify BACIC's standing as a prime location for warm cloud experimentation. The chamber has also been utilized to investigate effects of anthropogenic pollution over North China Plain (NCP) on cloud microphysics. Using ambient air and manipulating the expansion rate, a significant correlation is discovered between such pollution and the size distribution of cloud droplets. Interestingly, while an increase in aerosol leads to higher number of cloud droplets, it also causes a decrease in droplet size, typically within the range of 5-8 μm. Furthermore, an increase in aerosol number concentration leads to a decrease in the activation rate of aerosols into cloud droplets. This activation rate is around 10% for aerosol concentrations less than 5000 cm-3, and remains stable even when the aerosol concentration increases to 10000 cm-3.BACIC is also proved useful in conducting warm cloud expansion experiments involving different hygroscopic materials. It shows that the distribution of submicron (less than 1 μm) hygroscopic catalysts in a polluted environment leads to narrowing of the cloud droplet spectrum. It suggests that for the purpose of artificially reducing warm clouds or fog, it is recommended to use larger particle sizes. The results obtained from these diverse series of experiments have significantly contributed to theoretical knowledge and provide practical guidance for the ongoing development of artificial weather modification techniques.
Liquid water content (LWC) in clouds determines the precipitable water of clouds, which is a crucial factor for aircraft safety and weather modification operations. More importantly, it influences the optical depth of clouds in the visible wavelength range, thus determining their climate cooling effects. Identifying and quantifying the LWC in mixed-phase clouds via remote sensing techniques remains challenging owing to the large variability of hydrometeor sizes in the cloud. In this study, we used in-situ aircraft measured full size distributions and collocated airborne radar reflectivity (Z) to explicitly fractionate the contributions of hydrometeors (cloud liquid droplets, ice, and precipitation particles) at different size ranges from the measured total Z. A linearly decreasing contribution of non-precipitation hydrometeors with increasing total Z was discovered for a range of cloud types, including cumulus, status, and deep convection clouds. The relationship between the mass and Z for each type of hydrometeor derived from in situ measurements was then applied. This approach of apportioning the contribution of cloud liquid droplets from the measured total Z as the first step significantly reduced the scattering of the correlation between the LWC and Z, as presented in previous studies; thus, the LWC was more accurately determined. The derived liquid water path exhibited high agreement with the microwave radiometer measurements. Our method of deriving the LWC from the total Z stemming from the in situ measured size distributions may be applied in other situations to derive the cloud liquid droplets, ice, and precipitation masses for clouds with a given radar Z.
Ice-nucleating particles (INPs) are of great importance for regional weather and climate by altering the microphysical properties of clouds. Large uncertainties still exist for the sources, abundance and variability of INPs over the polluted North China Plain (NCP) due to limited observations in this region and the complex physical and chemical properties of aerosols from multiple sources. In this study, the concentrations of INPs in the immersion freezing mode at temperatures ranging from -5 ℃ to -30 ℃ were simultaneously measured for about one month in the Spring season. The measurements were carried out at a mountain site and a suburb site in Beijing representing clean and anthropogenic condition, respectively. Different concentrations and characteristics of INP are found for the two sites, which reflect the influence of different the air masses and INP sources. Consistent with previous studies in this region, dust particles are found to be the most abundant INPs during the Spring season, and the contribution from anthropogenic pollution aerosols was of minor importance. Most interestingly, the INP concentration at the mountain site was about one magnitude higher than at the suburban site at temperatures higher than -10 ℃, which is caused by the primary biological aerosol from the forests in the moutain area. Our results characterize the important role of these bioaerosols, which are also expected to have a strong impact on the glaciation of orographic clouds. In addition, to extend the data set, we investigated the characteristics of INPs in other seasons, to further study and quantify seasonal cycles of INP concentrations and sources.
Volatile organic compounds (VOCs) are precursors for ozone and secondary organic aerosol (SOA) formation, thereby playing a vital role in atmospheric chemistry and urban air quality. To characterize the relationship between VOCs and SOA, organics both in gas and particulate phases were concurrently measured in urban Beijing. The VOCs and organic aerosol (OA) were apportioned into factors with different oxidation levels by applying the factorization analysis on their detailed mass spectra. Six factors of VOCs were identified, including four primary VOCs (PVOC) factors and two secondary VOCs (SVOC) factors. The PVOC factors dominated the total VOCs when the air mass originated in the cleaner northern areas, while SVOC factors dominated for polluted southern air masses. The normalized concentrations of PVOC and primary OA factors showed consistent diurnal variations regardless of air mass directions, owing to the relatively stable local emissions during the experimental period. This contrasted with the secondary factors due to more complex transformation processes. The traffic-related VOCs and solid fuel combustion VOCs negatively correlated with SOA, implying that they may have contributed to the SOA formation through photooxidation. The VOCs in lower oxidation levels were found to have poor correlations with the less oxidized SOA, whereas they correlated strongly to the more oxidized SOA. This implied that the less oxidized SOA may be in a transition state, where its production and loss rates were balanced. These served as products of VOCs oxidation and reactants of more oxidized SOA formation, playing important roles on the VOC to SOA transformation. The identified VOC emission sources and their photochemical production of SOA should be considered in air quality policy planning.
The precipitation on the Tibetan Plateau, known as the water tower of Southeast Asia, is complex, especially in convective cloud precipitation. Many remote sensing and ground observations have been analyzed, but the insitu measurements of cloud microphysical characteristics are rare. Here we present aircraft observations of the microphysics of convective clouds over the Qinghai Tibet Plateau in China. These results show the microphysical structure of convective clouds and the triggering characteristics of precipitation in summer in Tibet. The vertical profile of July 9th was selected for a detailed analysis of microphysical characteristics. Mixed phase precipitation was initiated above the 7000 m above sea level over the TP, which is only about 500 m above cloud base height. Riming was the dominant precipitation forming process over the TP, leading to graupel formation, which was the primary form of precipitation of the convective clouds. Although the dust was a large fraction of the overall aerosols over the TP during the flights, it was not likely a major contribution to the early ice formation because of the temperature limit of the Ice Nuclei (IN) parameterization. The secondary ice process (SIP) appears to be the main source of ice crystals.
利用机载降水云雷达(Ka-band precipitation cloud radar,KPR)进行穿云观测,对KPR的数据质量进行以下研究:(1)由于KPR探测的原始数据存在很多背景噪声,对KPR的产品图采用高斯滤波进行去噪.(2)KPR的探测视角是以飞机为基准,为更好判断云顶、云底等信息,对KPR产品进行了飞机轨迹订正,并采用二次样条插值消除了飞机轨迹上的噪声和增益.(3)受飞机运动的影响,KPR测得的多普勒速度和频谱宽度与实际存在较大的误差,通过相关算法完成了多普勒速度和谱宽的订正.通过数据质量控制,KPR的产品质量得到明显改善.
Abstract. Aerosol-planetary boundary layer (PBL) interaction has been proposed as a key mechanism for stabilizing the atmosphere and exacerbating surface air pollution. Although the understanding of this process has progressed enormously, its magnitude and impact remain uncertain and vary widely concerning aerosol types, vertical distributions, synoptic conditions, etc. In this study, our primary interest is to distinguish the aerosol-PBL interaction of absorbing and scattering aerosols under contrasting synoptic patterns and aerosol vertical distributions. Detailed in-situ aircraft (KingAir-350) measurements and online coupled model Weather Research and Forecasting with Chemistry (WRF-Chem) simulations are explored over the North China Plain (NCP). Furthermore, a long-term PBL stability trend from 1980 to 2020 over the NCP is also investigated. The aircraft measurements and surface observations show that the surface air pollution over the Baoding City on 3 January is heavier than that on 4 January, 2020. In addition, the aerosols are restricted to the low layer on 3 January, whereas the aerosols mix more homogeneous upwards on 4 January. Thereupon, we focus on the two days with distinct synoptic circumstances, PBL stability, and aerosol vertical distributions over the NCP. According to the WRF-Chem modelling, the synoptic pattern over the Baoding City differs between the two days. The prevailing wind direction is opposite with a southwest wind on 3 January and a northeast wind on 4 January. The results indicate that the synoptic condition may affect the PBL thermal structure, thus affecting the aerosol vertical distribution. Additionally, the sensitive numerical experiments reveal that the light-absorbing and light-scattering aerosols have different effects on altering the PBL thermal structure. The inhibition effect of scattering aerosols on the PBL appears to be independent of the aerosol height distribution and solely depends on its concentration. However, aerosol-PBL feedback of absorbing aerosols is highly dependent on its vertical distribution. Our analysis highlights that we should principally concentrate on controlling the emissions of scattering aerosols under the stable stratification while cooperating to control the emissions of scattering and absorbing aerosols in an unstable stratification. Moreover, the long-term inter-annual variation in PBL stability shows a strong correlation with the East Asian Winter Monsoon, which seems to be valuable in determining which pollutants to target in different monsoon years and attaining more precise air pollution control. Based on the numerical simulations and observational constraints, a concept scheme description has been concluded to deepen our recognition of the interactions between thermodynamic stability and aerosols within the PBL over the NCP region.
In order to investigate the chemical composition and source apportionment of aerosols during winter in the Beijing-Tianjin-Heibei region, the particular matter (PM) and aerosol chemical composition at Mt. Haituo were observed by using a GRIMM 180, a single-particle soot photometer (SP2), and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) from December 28, 2020 to February 3, 2021. Combining these observations with meteorological data and the HYSPLIT model, we calculated the potential source contribution factor (PSCF) and concentration weighted trajectory (CWT) and analyzed the temporal evolution and potential sources apportionment of PM and aerosol chemical composition under different pollution processes. The results showed that the dust storm process mainly affected PM10 and PM2.5 in Mt. Haituo during the winter and had a small impact on PM1; by contrast, haze pollution mainly affected PM1. Chemical components of aerosol accounted for 85.0% and 73.4% of PM1 on clean and haze days, respectively, but only 47.4% of PM1 in dust storm processes. NO3- was the chemical component with the largest mass concentration in haze, accounting for 25.2% of PM1; black carbon (BC) had the largest mass concentration on clean and dust storm days, accounting for 24.1% and 12.8% of PM1, respectively. The median diameters of BC were 209.7, 207.5, and 204.7 nm on clean, dust storm, and haze days, respectively. Dp/Dc was 2.15 in haze pollution, which was 1.38 and 1.39 times that on dust storm and clean days, respectively. Diurnal variations in PM and aerosol chemical components were different during the different processes. PM10 and PM2.5had high mass concentrations at night and low mass concentrations during the daytime on clean and dust storm days and had a unimodal distribution with a peak at 14:00 in haze. Diurnal variations in chemical composition had a unimodal distribution on clean days and a bimodal distribution on dust storm and haze days. The chemical compositions of the BC coating layer were different under different processes. The coating layers of BC were mainly NH4NO3, (NH4)2SO4, and organic matter on the clean, dust storm, and haze days, respectively. The distribution of potential sources of PM1 and its chemical components were different under different processes. The high-value area of the potential sources was mainly concentrated in the Beijing-Baoding-Shijiazhuang-Yangquan area in the southwestern portion of the site during dust storms and was mainly concentrated in Yanqing, Huailai, and Changping in the areas around the site during haze.