Aerosol Sources Research Articles

Long-term change in winter aerosol composition and sources in Guiyang Southwest China (2003–2020)

This study presents a comprehensive analysis of air quality in China, Southwest China, over four winter seasons: 2003–2004, 2004–2005, 2017–2018 and 2019–2020. We initially collected Total Suspended Particles (TSP) samples during the earlier periods and PM2.5 samples during the later periods. Our goal was to illustrate the changes in sources of atmospheric pollutants over time. By focusing on the chemical composition of water-soluble inorganic ions (WSIIs), we highlighted significant long-term changes in air quality and pollution sources in Guiyang alongside the effectiveness of recent pollution treatment strategies. Historically affected by acid rain and acid pollution, Guiyang has shown notable improvements in air quality. Notably, sulfate pollution, primarily from coal combustion, has significantly decreased, with the sulfates concentration declining from an estimated 19.04 μg m−3 to 30.46 μg m−3 during the winter of 2003–2004, to just 7.37 μg m−3 in PM2.5 during the winter of 2019–2020. Additionally, the mean mass concentration of PM2.5 dropped by 18% between the 2017–2018 and 2019–2020 winters. An increasing ratio of nitrate to sulfate in the aerosols indicates a shift in pollution sources, with secondary nitrate pollution, largely from vehicle emissions, becoming increasingly prevalent. Positive Matrix Factorization (PMF) model analysis identified five major pollution sources, highlighting a transition from secondary sulfate to secondary nitrate as the primary contributors to air pollution in Guiyang, and secondary nitrate pollution mainly from vehicles emission was increasingly severe meanwhile the significance of ammonium should not be overlooked. The results stress the importance of local pollution sources and suggest a need for revised pollution control policies that address the evolving characteristics of aerosols and prioritize the major pollutants in Guiyang, especially during winter months.

Single particle characteristics and ice nucleation potential of particles collected during Asian dust storms in 2021

Dust storms have great impacts on air quality and climate. Dust can influence cloud microphysical properties and determine their radiative forcing and precipitation. Asian dust storms (ADS) are important sources of global aerosol. However, the physiochemical characteristics of dust from ADS at a single particle level are less understood, and the exact particles that can serve as ice nucleating particles (INPs) remain unclear. Here, we present the physicochemical properties and ice nucleation ability of dust particles collected in Beijing during two major ADS in March 2021. The particles from two ADS were classified into Illite, Kaolinite, Feldspar, Quartz, Chlorite, Mixed-dust, and Non-dust particles, which contributed 28.6 % ± 3.3 %, 20.0 % ± 3.9 %, 12.3 % ± 2.3 %, 11.1 % ± 2.8 %, 9.8 % ± 0.8 %, 13.7 % ± 1.8 %, and 4.4 % ± 1.7 % in number, respectively. On average, the ADS particles formed ice crystals via deposition ice nucleation from relative humidity with respect to ice (RHice) of 112 % ± 1 % at 250 K to 154 % ± 15 % RHice at 205 K. Part of the samples also formed ice via immersion freezing between 230 K and 250 K. Among the 149 identified INPs, Clay-like particles (Chlorite, Illite, and Kaolinite) contributed 71.1 % ± 6.2 % in number and followed by Mixed-dust-like particles (16.9 % ± 8.7 %) and Feldspar-like particles (10.4 % ± 6.3 %). Enrichment factor of each particle type in INPs is calculated as the ratio of its number fractions in INPs and the aerosol population. It ranges from 0.6 ± 0.7 to 1.3 ± 2.2. The contribution of each particle type to INP was correlated with its fraction in the population. These results imply that each particle type can serve as INP. Clay-like particles are the dominant INPs during the ADS. We conducted ice nucleation kinetic analysis and provided parameterizations of heterogeneous ice nucleation rate coefficient and contact angle for ADS. These parameterizations can be used in the modeling study to evaluate the impact of ADS in atmospheric ice crystal formation in clouds.

Drivers of PM2.5 Episodes and Exceedance in India: A Synthesis From the COALESCE Network

AbstractEmission sources influencing high particulate air pollution levels and related mortality in India have been studied earlier on country‐wide and sub‐national scales. Here, we use novel data sets of emissions (for 2019) and observations created under the Carbonaceous Aerosol Emissions, Source Apportionment, and Climate Impacts network in India (Venkataraman et al., 2020, https://doi.org/10.1175/bams‐d‐19‐0030.1) in WRF‐Chem simulations to evaluate drivers of high PM2.5 levels during episodes and in airsheds with different pollution levels. We identify airsheds in “extreme” (110–140 μg/m3), “severe” (80–110 μg/m3) and “significant” (40–80 μg/m3) exceedance of the Indian annual ambient air quality standard (National Ambient Air Quality Standards [NAAQS]) of 40 μg/m3 for PM2.5. We find that primary organic matter and anthropogenic mineral matter (largely coal fly‐ash) drive high PM2.5 levels, both annually and during high PM2.5 episodes. PM2.5 episodes are driven by organic aerosol in north India (Mohali) in wintertime but are additionally influenced by mineral matter and secondary inorganics in central (Bhopal), south India (Mysuru) and eastern India (Shyamnagar). Across airsheds in exceedance of the NAAQS and during high PM2.5 episodes, primary PM2.5 emissions arise largely from the residential sector (50%–75%). Formal sector emissions (industry, thermal power and transport; 40%–55%) drive airshed and episode scale PM2.5 exceedance in northern and eastern India. Agricultural residue burning emissions predominate (50%–75%) on episode scales, both in northern and central India, but not on annual scales. Interestingly, residential sector emissions strongly influence (60%–90%) airsheds in compliance with the NAAQS (annual mean PM2.5 < 40 μg/m3), implying the need for modern residential energy transitions for the reduction of ambient air pollution across India.

Composition and Sources of Organic Aerosol in Two Megacities in Western China Using Complementary Mass Spectrometric and Statistical Techniques.

Over 300 daily PM2.5 filter samples were collected in two western Chinese megacities, Xi'an and Chongqing, from October 2019 to May 2020. Their aqueous extracts were nebulized simultaneously to an aerosol mass spectrometer (AMS) and a recently developed extractive electrospray ionization (EESI) mass spectrometer, for bulk and near-molecular organic aerosol (OA) composition, respectively. Carbonate was quantified using EESI and a total organic carbon analyzer to separate inorganic carbon from dust. Via isotopically-labelled internal standards and positive matrix factorization, seven water-soluble sources were quantified separately using the AMS- and EESI-based analyses, with consistent types, concentrations, and correlations. These include dust, solid fuel combustion (SFC)-related, nitrogen- (and sulfur-) containing, summer/winter oxygenated OAs, and a cigarette-related OA only in EESI. When accounting for water-solubility, SFC-related OAs were the largest (53%) sources in Chongqing, while dust (consisting of 77% OA and 23% carbonates) was the largest (30%) source in Xi'an. Overall, this study presents one of the first times that complementary mass spectrometric techniques independently resolved consistent OA sources-with added chemical information-over multiple seasons and locations of complex pollution. The methods and quantified sources are essential for subsequent chemical, modelling, and health studies, and policy making for air pollution mitigation.

Estimating black carbon levels using machine learning models in high-concentration regions

Black carbon (BC) is emitted into the atmosphere during combustion processes, often in conjunction with emissions such as nitrogen oxides (NOx) and ozone (O3), which are also by-products of combustion. In highly polluted regions, combustion processes are one of the main sources of aerosols and particulate matter (PM) concentrations, which affect the radiative budget. Despite the high relevance of this air pollution metric, BC monitoring is quite expensive in terms of instrumentation and of maintenance and servicing. With the aim to provide tools to estimate BC while minimising instrumentation costs, we use machine learning approaches to estimate BC from air pollution and meteorological parameters (NOx, O3, PM2.5, relative humidity (RH), and solar radiation (SR)) from currently available networks. We assess the effectiveness of various machine learning models, such as random forest (RF), support vector regression (SVR), and multilayer perceptron (MLP) artificial neural network, for predicting black carbon (BC) mass concentrations in areas with high BC levels such as Northern Indian cities (Delhi and Agra), across different seasons. The results demonstrate comparable effectiveness among the models, with the multilayer perceptron (MLP) showing the most promising results. In addition, the comparability between estimated and monitored BC concentrations was high. In Delhi, the MLP shows high correlations between measured and modelled concentrations during winter (R2: 0.85) and post-monsoon (R2: 0.83) seasons, and notable metrics in the pre-monsoon (R2: 0.72). The results from Agra are consistent with those from Delhi, highlighting the consistency of the neural network's performance. These results highlight the usefulness of machine learning, particularly MLP, as a valuable tool for predicting BC concentrations. This approach provides critical new opportunities for urban air quality management and mitigation strategies and may be especially valuable for megacities in medium- and low-income regions.

Distribution Characteristics and Source Analysis of Carbonaceous Aerosols Before and After the Spring Festival in the Guanzhong Plain

The spatio-temporal variation characteristics and potential sources of carbonaceous aerosols in the Guanzhong Plain during the Spring Festival in 2023 were analyzed using inverse distance weighting spatial interpolation （IDW）, secondary organic carbon （SOC） estimation, and potential source contribution factor analysis （PSCF）, with the OC and EC in the PM2.5 of five cities： Xi'an, Baoji, Xianyang, Weinan, and Tongchuan as the research objects. The results showed that in terms of time distribution, ρ（OC） was as follows： after the Spring Festival [（18.6 ±11.0） μg·m-3] &gt; during the Spring Festival [（16.2 ±15.1） μg·m-3] &gt; before the Spring Festival [（10.0 ±8.3） μg·m-3], and ρ（EC） was as follows： after the Spring Festival [（2.2 ±1.2） μg·m-3] &gt; during the Spring Festival [（1.7 ±1.5） μg·m-3] &gt; before the Spring Festival [（1.4 ±1.1） μg·m-3], which indicated that OC and EC concentrations were the most severe after the Spring Festival. In terms of spatial distribution, ρ（OC） was as follows： Xianyang [（21.4 ±17.3） μg·m-3] &gt; Baoji [（15.8 ±12.8） μg·m-3] &gt; Xi'an [（13.6 ±11.3） μg·m-3] &gt; Weinan [（11.6 ±9.1） μg·m-3] &gt; Tongchuan [（10.0 ±8.3） μg·m-3], and ρ（EC） was as follows： Xianyang [（2.1 ±1.4） μg·m-3] &gt; Weinan [（1.8 ±1.4） μg·m-3] &gt; Xi'an [（1.8 ±1.2） μg·m-3] &gt; Tongchuan [（1.6 ±1.4） μg·m-3] &gt; Baoji [（1.2 ±0.9） μg·m-3]. Overall, Xianyang had the most severe PM2.5 and carbon aerosol pollution, whereas Tongchuan had the least pollution. IDW results showed that the high-value center of OC and EC concentration [ρ（OC） &gt; 27.3 μg·m-3, ρ（EC） &gt; 2.9 μg·m-3] was in the middle of the plain, the low-value center of OC and EC concentration [ρ（OC） <7.0 μg·m-3, ρ（EC） < 1.0 μg·m-3] was in the northern plain, and the distribution of OC was higher in the west and lower in the east, whereas the distribution of EC was higher in the east and lower in the west. The proportion of SOC in OC was as follows： after the Spring Festival （51.7%） &gt; during the Spring Festival （41.1%） &gt; before the Spring Festival （36.8%）. The SOC/OC values of each city and the contribution rate of SOC of each city to the Guanzhong Plain indicated that Tongchuan, Baoji, and Xianyang were greatly affected by the secondary conversion of organic carbon. The correlation of OC and EC before, during, and after the Spring Festival （r = 0.85, r = 0.98, and r = 0.94, respectively） indicated a high degree of homology between them. Carbonaceous aerosols had a certain correlation with humidity and wind speed before and during the Spring Festival but had a weak correlation with meteorological factors after the Spring Festival. Carbonaceous aerosols generally were strongly correlated with CO and NO2, and the correlation was strongest after the Spring Festival, whereas the correlation with SO2 was strongest during the Spring Festival. The potential source areas of carbonaceous aerosols in the five cities were mainly concentrated in the local and surrounding areas of southern Gansu, northern Shaanxi, and southern Shaanxi. They were also affected by long-distance transportation from the northwest before the Spring Festival.

Compositions and sources of fluorescent water-soluble and water-insoluble organic aerosols

Brown carbon (BrC), the light-absorbing component of organic aerosols, plays a significant role in climate change and atmospheric photochemistry. However, the water-insoluble fractions of BrC have not been extensively studied, limiting the assessment of the overall climate effects of BrC. In this study, water-soluble and -insoluble organic carbon (i.e., WSOC and WIOC) in wintertime aerosols in Hefei were subsequently fractionated, and their fluorescence properties were comparatively investigated with the excitation–emission matrix method. WIOC contributing 57.1 % was the major component of organic carbon. WSOC with the largest contribution from humic-like regions exhibited a redshift compared to WIOC. Three humic-like substances (HULIS) with different oxidation degrees and one protein-like substances (PRLIS) were identified as the major fluorescent components by the parallel factor analysis. WSOC had more highly oxygenated HULIS, whereas low-oxygenated HULIS dominated WIOC. Nighttime WIOC contained more less-oxygenated species. The positive matrix factorization analysis suggested that biomass burning (43 %) was the largest source of both fluorescent WSOC and WIOC. Coal combustion contributed much more to fluorescent WIOC (40 %), whereas secondary formation contributed more to fluorescent WSOC (12 %). During aerosol pollution episodes, the increase in fluorescence efficiency was much greater for WIOC (25 %) than for WSOC (12 %), and WSOC and WIOC experienced a redshift and blueshift in emission wavelength, respectively. WSOC had more highly oxygenated HULIS, while WIOC had more less-oxygenated HULIS in aerosol episodes than the non-episodic periods. In addition, aerosol pollution was accompanied by the increased contributions of biomass burning and coal combustion to both fluorescent WSOC and WIOC, while the decreased relative contribution of secondary formation to fluorescent WSOC. Our findings highlighted the different fluorescence properties, compositions and sources of fluorescent WSOC and WIOC, providing a comprehensive view of BrC aerosols.

Dust Events over the Urmia Lake Basin, NW Iran, in 2009–2022 and Their Potential Sources

Nowadays, dried lake beds constitute the largest source of saline dust storms, with serious environmental and health issues in the surrounding areas. In this study, we examined the spatial–temporal distribution of monthly and annual dust events of varying intensity (dust in suspension, blowing dust, dust storms) in the vicinity of the desiccated Urmia Lake in northwestern (NW) Iran, based on horizontal visibility data during 2009–2022. Dust in suspension, blowing dust and dust storm events exhibited different monthly patterns, with higher frequencies between March and October, especially in the southern and eastern parts of the Urmia Basin. Furthermore, the intra-annual variations in aerosol optical depth at 500 nm (AOD550) and Ångström exponent at 412/470 nm (AE) were investigated using Terra/Aqua MODIS (Moderate Resolution Imaging Spectroradiometer) data over the Urmia Lake Basin (36–39°N, 44–47°E). Monthly distributions of potential coarse aerosol (AE &lt; 1) sources affecting the lower troposphere over the Urmia Basin were reconstructed, synergizing Terra/Aqua MODIS AOD550 for AE &lt; 1 values and HYSPLIT_4 backward trajectories. The reconstructed monthly patterns of the potential sources were compared with the monthly spatial distribution of Terra MODIS AOD550 in the Middle East and Central Asia (20–70°E, 20–50°N). The results showed that deserts in the Middle East and the Aral–Caspian arid region (ACAR) mostly contribute to dust aerosol load over the Urmia Lake region, exhibiting higher frequency in spring and early summer. Local dust sources from dried lake beds further contribute to the dust AOD, especially in the western part of the Urmia Basin during March and April. The modeling (DREAM8-NMME-MACC) results revealed high concentrations of near-surface dust concentrations, which may have health effects on the local population, while distant sources from the Middle East are the main controlling factors to aerosol loading over the Urmia Basin.

Natural and anthropogenic sources of organic aerosol in the atmosphere: kinetics and mechanism of formation in the forest-steppe zone of Western Siberia

Natural and anthropogenic sources of organic aerosol in the atmosphere: kinetics and mechanism of formation in the forest-steppe zone of Western Siberia

Large contribution of in-cloud production of secondary organic aerosol from biomass burning emissions

Organic compounds released from wildfires and residential biomass burning play a crucial role in shaping the composition of the atmosphere. The solubility and subsequent reactions of these compounds in the aqueous phase of clouds and fog remain poorly understood. Nevertheless, these compounds have the potential to become an important source of secondary organic aerosol (SOA). In this study, we simulated the aqueous SOA (aqSOA) from residential wood burning emissions under atmospherically relevant conditions of gas-liquid phase partitioning, using a wetted-wall flow reactor (WFR). We analyzed and quantified the specific compounds present in these emissions at a molecular level and determined their solubility in clouds. Our findings reveal that while 1% of organic compounds are fully water-soluble, 19% exhibit moderate solubility and can partition into the aqueous phase in a thick cloud. Furthermore, it is found that the aqSOA generated in our laboratory experiments has a substantial fraction being attributed to the formation of oligomers in the aqueous phase. We also determined an aqSOA yield of 20% from residential wood combustion, which surpasses current estimates based on gas-phase oxidation. These results indicate that in-cloud chemistry of organic gases emitted from wood burning can serve as an efficient pathway to produce organic aerosols, thus potentially influencing climate and air quality.

Characteristics and Sources of Organic Aerosol in PM2.5 at Yangbajing in Tibetan Plateau

The climate and environment of the Tibetan Plateau (TP) are sensitive to human activities. As a key component highly influencing global climate and environment, organic aerosol over the TP is investigated in this study, especially in organic composition and its sources. This study aims to explore the composition characteristics, seasonal variation, and potential sources of organic aerosol including two episodes through one-year sampling at the Yangbajing (YBJ) site in the TP. A total of 120 primary and secondary organic species as well as organic carbon (OC) and elemental carbon (EC) were measured in PM2.5. The annual average concentrations of OC, EC, and organic species were 3.12 ± 3.73 μgC/m3, 0.28 ± 0.18 μgC/m3 and 104 ± 36.6 ng/m3, respectively. High ratio of OC to EC (OC/EC) and low ratio of fatty acids to n-alkanes were found for aerosol in the TP. The OC/EC ratio was 11.8 ± 10.2 on average at the YBJ site and strongly correlated with levoglucosan, a tracer for biomass burning, but not so with typical secondary species, indicating that the high ratio of OC/EC over the TP was more influenced by biomass burning than secondary formation. The ratio of fatty acids to n-alkanes at YBJ was 1.39 ± 0.29 on average, lower than those reported over urban areas (3.13 ± 1.49), probably owing to less residential cooking activities. Seasonally, the non-monsoon season had significant increases in primary organic aerosol (POA) tracers, among which biomass burning tracers had a higher increase percentage than other specific tracers. On the contrary, the levels of secondary organic aerosol (SOA) tracers, especially isoprene- and monoterpene-derived SOA tracers were enhanced in the monsoon season (summer time), largely resulting from high emissions of biogenic volatile organic compounds. Two episodes characterized with much higher concentrations of organic species (1215 and 688 ng/m3) were observed in this study. One was characterized by significant enhancement of POA tracers with the air masses originated from South Asia, and the other showed large increases in SOA and POA tracers with the air masses transported across multiple regions. This study could help to better understand the influence of human activities on atmospheric organic aerosol in remote regions and how POA and SOA vary with seasons and in different episodes.

Characterization and sources of carbonaceous aerosol in ambient PM1 in Qingdao, a coastal megacity of northern China from 2017 to 2022

Organic carbon (OC) and elemental carbon (EC) are major chemical constituents of ambient submicron particles (PM1) and have substantial implications for air quality, climate dynamics, and human health. Long-term observations of daily mean mass concentrations of OC and EC in PM1 were conducted in Qingdao, a typical coastal megacity in northern China, in autumn and winter from Nov. 2017 to Jan. 2023. The variety in OC and EC concentrations under the active emission reduction policies of long-term carbon reduction in China, combined with the impact of the COVID-19 pandemic, were analyzed. OC and EC concentrations decreased noticeably from 8.28 ± 4.59 μg m−3 and 2.00 ± 1.17 μg m−3 during pre-COVID-19 pandemic to 6.34 ± 3.82 μg m−3 and 1.87 ± 1.01 μg m−3 during post-COVID-19 pandemic, respectively. The XGBoost-SHAP model indicated that emission sources had the most significant effect on OC and EC concentrations, followed by meteorological factors. Unfavorable meteorological conditions and a substantial increase in emissions are responsible for the increase of OC and EC concentration in winter. Potential source contribution function results indicated that the southern, eastern, and central Shandong regions were the primary source areas for transporting high concentrations of carbonaceous components. Positive matrix factorization analysis suggested that carbonaceous aerosols in Qingdao predominantly originated from coal/biomass combustion (54.75%–81.78%) and local vehicle emissions (8.72%–28.73%). Compared with that before COVID-19, coal/biomass combustion's contribution to OC and EC decreased by 19% after the COVID-19 pandemic. The contribution of vehicles increased by 110%, possibly due to the increase in motor vehicles and the rapid recovery in diesel consumption in freight transportation. Prohibiting biomass burning, such as open burning of straw, and measures such as promoting low-carbon and clean production of coal-fired industrial furnaces might have played a key role in reducing OC and EC levels. These results contribute to a deeper understanding of the concentration levels and sources of carbonaceous components in PM1 and provide theoretical guidance for environmental management.

Origins of the seasonal variability of PM2.5 sources in a rural site in Northern France

Air quality in rural areas results from the crossing of aged air masses transported from urban areas with local emissions dominated by agriculture and vegetation. The result is a complex mixture of primary and secondary atmospheric species, coming from varied sources and geographical areas. We implemented a methodology for deconvoluting and determining the geographical origins of the main aerosol sources impacting a typical rural area of northern France. A one-year field campaign was conducted in a rural site located between Paris and Brussels from March 2018 to February 2019. Hourly-based observations of inorganic and organic precursor gases and PM2.5 speciation were collected using on-line instrumentation. The annual PM2.5 concentrations of 12.2 ± 9.23 μg m−3 were explained by four sources extracted through positive matrix factorization analyses: combustion (40.2%), NO3-rich (26.8%), SO4-rich (18%) and mixed aged marine (15%). The combustion and SIA-rich sources drive 85 % of the yearly PM2.5 mass and variability. The combustion factor was most prominent during winter (53.3% of PM2.5 mass) due to high contributions from local and regional transport of biomass burning pollutants (winter OC/EC = 6.0; OC-to-OM factor = 2.05). In summer, it was most likely driven by secondary organic aerosol production and agricultural waste burning events (summer OC/EC = 8.6; OC-to-OM factor = 1.85). Comparing with other regional sites, we observed a strong regional background of carbonaceous particles regardless of the site typology. The SIA fraction is dominated by the NO3-rich source compared to the SO4-rich source. In spring, NO3-rich particles dominate PM2.5 (36.9%) due to intense agricultural activity. The temporal variability is driven by transport processes from the Benelux area in a North-to-South gradient of decreasing concentrations. A minor proportion of the NH4NO3 observed seems to be due to the local effects of morning dew and photochemical oxidation of NO2 in the afternoon. HNO3 appears to be the limiting factor for local NH4NO3 formation. PM2.5 toxicity in rural areas with low population densities should be not only addressed based on mass concentration, but also considering the chemical composition of particles as people from rural environments are exposed to high contributions from biomass burning sources and secondary inorganic aerosols triggered by the NH3 excess.

Aerosol sources and transport paths co-control the atmospheric bacterial diversity over the coastal East China Sea

Airborne bacteria along with chemical composition of aerosols were investigated during five sampling seasons at an offshore island of the East China Sea. Bacterial diversity was the lowest in spring, the highest in winter, and similar between the autumns of 2019 and 2020, suggesting remarkably seasonal variation but little interannual change. Geodermatophilus (Actinobacteria) was the indicator genus of mineral dust (MD) showed higher proportion in spring than in other seasons. Mastigocladopsis_PCC-10914 (Cyanobacteria) as the indicator of sea salt (SS) demonstrated the highest percentages in both autumns, when the air masses mainly passed over the ocean prior to the sampling site. The higher proportions of soil-derived genera Rubellimicrobium and Craurococcus (both Proteobacteria) and extremophile Chroococcidiopsis_SAG_2023 (Cyanobacteria) were found in summer and winter, respectively. Our study explores the linkage between aerosol source and transport path and bacterial composition, which has implication to understanding of land-sea transmission of bacterial taxa.

Investigating the convective transport possibilities of lower-atmospheric pollutants to the UTLS region using rainwater and aerosol chemical characterization

Various attempts using different platforms to understand the chemical composition of the Asian Tropopause Aerosol Layer (ATAL) have concluded that it primarily consists of nitrate (NO3−) aerosols. Recent in-situ measurements from aircraft flying through ATAL have suggested that ammonia (NH3) pollution from Asia could serve as the precursor for nitrate aerosols in ATAL through gas-to-particle formation after undergoing convective uplift to the Upper Troposphere and Lower Stratosphere (UTLS) regions. In this study, we aimed to investigate the potential pathways of convective transport of lower-atmospheric pollutants by analysing the chemical composition of rainwater and aerosols in a highly convective region, Kolkata (Head Bay of Bengal), India. We utilized the PILS-IC system established at Kolkata Camp Observatory of the National Atmospheric Research Laboratory (KCON). The analysis revealed a significant dominance of NH4+ and NO3− ions in both rainwater and aerosol samples during the monsoon and post-monsoon seasons, with the dominance increasing during the post-monsoon season. Air mass trajectories indicated a clear influence of the Indo-Gangetic Plain (IGP) region during the post-monsoon season, which is well-known for its dense agricultural activities and industries. High concentrations of NH3 even at higher altitudes, have been observed in Atmospheric Infrared Sounder (AIRS) measurements. Moreover, using Outgoing Longwave Radiation (OLR) and vertical wind as proxies for tropical deep convection and updrafts/downdrafts, respectively, we found evidence supporting the possibility of convective transport of these lower-atmospheric pollutants to the UTLS regions during the monsoon season. In conclusion, this study provides evidence for the potential convective transport of lower-atmospheric pollutants, including NH3 and other precursor gases, to higher levels. These pollutants could partially serve as the source of nitrate aerosols in the ATAL through gas-to-particle formation processes.

Regional Aerosol Optical Depth over Antarctica

Atmospheric aerosols greatly contribute to the uncertainty in current climate models, particularly presenting pronounced limitations in the Antarctic region. This study measures aerosol properties using data from several Antarctic AERONET sites (Escudero, Marambio, South Pole, Utsteinen, Vechernaya_Hill) and Zhongshan Station. We examined the spatial and temporal patterns of two specific aerosol properties: Aerosol Optical Depth (AOD) at 500 nm (τ500nm) and Ångström Exponent (AE) between 440 and 870 nm (α440−870nm). Our findings reveal τ500nm medians ranging from 0.02 to 0.09, with elevated values observed along the coastal regions compared to the interior of Antarctica. Regarding the AE, the medians of α440−870nm indicate that the coarse-mode particle aerosols are dominated at Escudero (approximately 0.54). In contrast, fine mode particles prevail at the other sites (over 0.97). Monthly mean τ500nm and the proportion of fine mode particles peaks during austral summer and autumn, suggesting increased marine biological sources. Moreover, analyzing the air mass back trajectories, we discovered marine air influences on Escudero, Marambio, Zhongshan, and Vechernaya_Hill, while Utsteinen and South Pole are primarily experiencing air originating from the Antarctic continent. These findings underscore the significant role of aerosol sources in regional AOD differences. Additionally, higher τ500nm were more associated with significantly negative direct aerosol radiative forcing at the bottom of the atmosphere (DARF-BOA). The direct aerosol radiative forcing at the top of the atmosphere (DARF-TOA) closely correlates with single-scattering albedo (SSA), where high (low) SSA generally results in negative (positive) forcing over Antarctica.

Characteristics of Cloud and Aerosol Derived from Lidar Observations during Winter in Lhasa, Tibetan Plateau

In order to investigate the variations of cloud and aerosol vertical profiles over the Tibetan Plateau (TP) in winter, we performed ground-based lidar observations in Lhasa, a city on the TP, from November 2021 to January 2022. The profiles of extinction coefficient, depolarization ratio, and signal-to-noise ratio (SNR) were retrieved using the atmospheric echo signals collected by the lidar. Clouds were identified by the range-correction echo signals and classified into water clouds, mixed clouds, horizontally oriented ice crystal clouds (HOICC), and ice clouds by the depolarization ratio and the hourly temperature from the European Centre for Medium-Range Weather Forecasts Reanalysis version 5 (ERA5). The clouds mainly appeared at a height of 3~5 km from 14:00–22:00 Beijing Time throughout the field campaign. The height and frequency (~30%) for cloud appearance were significantly lower than that reported in previous studies in summer. The cloud categories were dominated by mixed clouds and ice clouds during the observation period. The proportions of ice clouds gradually increased with increasing heights. After eliminating profiles influenced by clouds, the aerosol extinction coefficient and depolarization ratio were obtained, and the atmospheric boundary layer height (ABLH) was calculated. The aerosol extinction coefficient decreased with increasing height in the ABLH, and there were no obvious changes for the aerosol extinction coefficient above the ABL. The aerosol extinction coefficients near the Earth’s surface presented two peaks, appearing in the morning and evening, respectively. The high aerosols at the surface in the morning continually spread upward for 4–5 h and finally reached an altitude of 1 km with the development of ABLH. In addition, the depolarization ratio of aerosols decreased slowly with increasing altitudes. There was no obvious diurnal variation for depolarization ratios, indicating partly that the source of aerosols did not change significantly. These results are beneficial in understanding the evolution of cloud and aerosol vertical profiles over the TP.

Three-Dimensional Structure and Transport Properties of Dust Aerosols in Central Asia—New Insights from CALIOP Observations, 2007–2022

Central Asia (CA) is one of the major sources of global dust aerosols. They pose a serious threat to regional climate change and environmental health and also make a significant contribution to the global dust load. However, there is still a gap in our understanding of dust transport in this region. Therefore, this study utilizes Cloud–Aerosol LiDAR with Orthogonal Polarization (CALIOP) data from 2007 to 2022 to depict the three-dimensional spatiotemporal distribution of dust aerosols over CA and to analyze their transport processes. In addition, the Tropospheric Monitoring Instrument (TROPOMI) was employed to assist in monitoring the movement of typical dust events, and the trajectory model was utilized to simulate the forward and backward trajectories of a dust incident. Additionally, a random forest (RF) model was employed to rank the contributions of various environmental factors. The findings demonstrate that high extinction values (0.6 km−1) are mostly concentrated within the Tarim Basin of Xinjiang, China, maintaining high values up to 2 km in altitude, with a noticeable decrease as the altitude increases. The frequency of dust occurrences is especially pronounced in the spring and summer seasons, with dust frequencies in the Tarim Basin and the Karakum and Kyzylkum deserts exceeding 80%, indicating significant seasonal and regional differences. The high values of dust optical depth (DOD) in CA are primarily concentrated in the summer, concurrent with the presence of a stable aerosol layer of dust in the atmosphere with a thickness of 0.62 km. Furthermore, dust from CA can traverse the Tianshan mountains via the westerlies, transporting it eastward. Additionally, skin temperature can mitigate regional air pollution. Our results contribute to a deeper understanding of the dynamic processes of dust in CA and provide scientific support for the development of regional climate regulation strategies.

Chemical composition, source characteristics, and hygroscopic properties of organic-enriched aerosols in the high Arctic during summer

Arctic regions are extremely sensitive to global warming. Aerosols are one of the most important short-lived climate-forcing agents affecting the Arctic climate. The present study examines the summertime chemical characteristics and potential sources of various organic and inorganic aerosols at a Norwegian Arctic site, Ny-Ålesund (79°N). The results show that organic matter (OM) accounts for 60 % of the total PM10 mass, followed by sulfate (SO42−). Water-soluble organic carbon (WSOC) contributes 62 % of OC. Photochemical processes involving diverse anthropogenic and biogenic precursor compounds are identified as the major sources of WSOC, while water-insoluble organic carbon (WIOC) aerosols are predominantly linked to primary marine emissions. Despite being a remote pristine site, the aerosols show a sign of chemical aging, evidenced by a significant chloride depletion, which was about 82 % on average during the study period. Nitrogen-containing aerosols are likely stemming from migratory seabird colonies and local dust sources around the sampling site. While biogenic, crustal, and sea salt-derived SO42- account for 37%, 8%, and 5% respectively, the remaining 50% is attributed to anthropogenic SO42-. Through chemical tracers, Pearson correlation coefficient matrix, and Hierarchical Cluster Analysis (HCA), the present study identifies soil biota (terrestrial biogenic) and marine emissions, along with their photochemical oxidation processes, as potential sources of Arctic aerosols during summer, while biomass burning and combustion-related sources have a minor contribution. The chemical closure of hygroscopicity highlights that while organics predominantly control aerosol hygroscopicity in the Arctic summer, specific inorganic components like (NH4)2SO4 can significantly increase it on certain days, affecting aerosol-cloud interactions and climate processes over the Arctic during summer. The present study highlights the high abundance of organics and their vital role in the Arctic climate during summer when natural aerosols are conquered.

Global source apportionment of aerosols into major emission regions and sectors over 1850–2017

Abstract. Anthropogenic emissions of aerosols and precursor gases have changed significantly in the past few decades around the world. In this study, the Explicit Aerosol Source Tagging (EAST) system is merged into the Energy Exascale Earth System Model version 1 (E3SMv1) to quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions across the globe during 1850–1980, 1980–2010, and 2010–2017. In North America and Europe, changes in anthropogenic PM2.5 were mainly caused by changes in emissions from local energy and industrial sectors. The local industrial sector caused the largest increase in PM2.5 in East Asia during 1980–2010 and decrease during 2010–2017. In South Asia, the increase in energy-related emissions dominated the rise in PM2.5 levels during 1980–2017. During 1850–1980, the increases in emissions from North America contributed to the increase in the European PM2.5 burden by 1.7 mg m−2 and the sources from the Europe were also responsible for the PM2.5 burden increase in East Asia and South Asia by about 1.0 mg m−2. During 1980–2010, East Asia contributed to an increase of 0.4–0.6 mg m−2 in the PM2.5 burden in North America and Europe, while South Asia contributed about 0.3 mg m−2. During 2010–2017, the contributions from East Asia to the PM2.5 burdens in the North America, Europe, and South Asia declined by 0.3–0.6 mg m−2 due to the clean air actions in China, while the contributions from South Asia still increased due to the continuous increase in emissions in South Asia. The historical changes in aerosols had an impact on effective radiative forcing through aerosol–radiation interactions (ERFari). During 1980–2010, a decline in North American aerosols resulted in a positive ERFari change (warming effect) in Europe and a decline in aerosols in Europe caused a warming effect in Russia and northern China. The changes in ERFari from the increase and decrease in aerosols in China during 1980–2010 and 2010–2017, respectively, are comparable in magnitude. The continuous aerosol increases in South Asia from 1980 to 2017 resulted in negative ERFari (cooling) changes in South Asia, Southeast Asia, and southern China.