Aerosol Characteristics Research Articles

Vertical Profiles of Aerosols Induced by Dust, Smoke, and Fireworks in the Cold Region of Northeast China

Despite the long-term implementation of air pollution control policies in northeast China, severe haze pollution continues to occur frequently. With the adoption of a megacity (Changchun) in northeast China, we analysed the vertical characteristics of aerosols and the causes of aerosol pollution throughout the year using multisource data for providing recommendations for controlling pollution events (i.e., straw burning and fireworks). Based on a ground-based LiDAR, it was found that the extinction coefficient (EC) of aerosols at a height of 300 m in Changchun was highest in winter (0.44 km−1), followed by summer (0.28 km−1), with significant differences from those in warmer regions, such as the Yangtze River Delta. Therefore, it is recommended that air pollution control policies be differentiated between winter and summer. On Chinese New Year’s Eve in Changchun, the ignition of firecrackers during the day and night caused increases in the EC at a height of 500 m to 0.37 and 0.88 km−1, respectively. It is suggested that the regulation of firecracker ignition should be reduced during the day and strengthened at night. Based on the CALIPSO and backward trajectory analysis results, two events of dust–biomass-burning composite pollution were observed in March and April. In March, the primary aerosol component was dust from western Changchun, whereas in April, the main aerosol component was biomass-burning aerosols originating from northern and eastern Changchun. Hence, reducing the intensity of spring biomass burning can mitigate the occurrence of dust–biomass-burning composite pollution. These findings can provide emission policy suggestions for areas facing similar issues regarding biomass-burning transmission pollution and firework emissions.

Optical and physical characteristics of aerosols over Asia: AERONET, MERRA-2 and CAMS

A comprehensive study on the regional and spatial distributions of aerosol columnar optical and physical characteristics utilizing high-quality Aerosol Robotic Network (AERONET) datasets over Asia (Central, South, South-East, and East Asia), along with spatiotemporal collocated validation of two highly-spatially resolved models (Modern-Era Retrospective Analysis for Research and Applications-2 (MERRA-2) and Copernicus Atmosphere Monitoring Service (CAMS)) simulated aerosol optical depth (AOD) and Ångström exponent (AE) on annual and seasonal scales, is conducted for the first time. AOD is the highest over South Asia in each season, followed by South-East, East, and Central Asia. Annual regional average AOD at 0.50 μm over South Asia is 0.61. Combined influence of both fine mode anthropogenic aerosol emissions from fossil fuel combustion and biomass burning, and coarse mode dust aerosols from seasonal transport lead to higher AOD and total volume concentration (TVC), and exhibit significant spatiotemporal variations. Coarse volume fraction (CVF) and effective radius (Reff) are higher over Central Asia due to the dominance of coarse dust aerosols. East and South-East Asia are dominated by fine mode aerosols and result in higher fine volume concentration (FVC), AE, fine mode fraction (FMF), and lower Reff. Compared to the other regions of the globe (except Africa), AOD is higher over Asia, with higher spatiotemporal variabilities in AOD, AE, FMF, and TVC. Over Asia, the agreement between AERONET and CAMS AOD is better than that of AERONET and MERRA-2 AOD. For high AOD conditions, underestimation in model AODs is higher, and lower fraction of model AODs satisfy the Global Climate Observing System (GCOS) requirement over all regions, and these are more pronounced over Asia. Biases in model AODs are higher over Asia compared to the other regions of the globe, and lower over North America, Europe, and Australia. Higher bias in model AEs compared to AODs over all the regions shows substantial challenges in simulating spectral AOD and appropriate contributions of fine and coarse mode aerosols. These findings over a global aerosol hotspot region, Asia, along with other regions of the globe are crucial for accurate simulation and fine-tuning of aerosol characteristics by regional and global models, and for reducing uncertainties in the assessment of radiative and climate impact of aerosols.

Measurement of Aerosol Transmission Through a Stress Corrosion Crack–Like Geometry

The formation of a stress corrosion crack (SCC) in the canister wall of a dry cask storage system (DCSS) has been identified as a potential issue for the long-term storage of spent nuclear fuel. The presence of a SCC in a storage system could represent a through-wall flow path from the canister interior to the environment. Modern, vertical DCSSs are of particular interest due to the commercial practice of using relatively high helium backfill pressures (up to approximately 800 kPa) in the canister to enhance internal natural convection. This pressure differential offers a comparatively high driving potential for blowdown of any particulates that might be present in the canister in the event of a through-wall SCC. In this study, the rates of gas flow and aerosol transmission of a spent fuel surrogate through an engineered microchannel with dimensions representative of a SCC were evaluated experimentally using coupled mass flow and aerosol analyzers. The microchannel was formed by mating two gauge blocks with a linearly tapering slot orifice nominally 13 μm (0.0005 in.) tall on the upstream side and 25 μm (0.001 in.) tall on the downstream side. The orifice is 12.7 mm (0.500 in.) wide by 8.89 mm (0.350 in.) long (flow length). Surrogate aerosols of cerium oxide (CeO2) were seeded and mixed with either helium or air inside a pressurized tank. The aerosol characteristics were measured immediately upstream and downstream of the simulated SCC at elevated and ambient pressures, respectively. The next iteration of testing involves replacing the engineered microchannel with lab-grown SCCs. Preliminary clean flow testing has been conducted on SCC samples provided by the Electric Power Research Institute. These data sets demonstrate a new capability to characterize SCCs under well-controlled boundary conditions. Preliminary testing efforts are focused on understanding the evolution in both the size and quantity of a hypothetical release of aerosolized spent fuel particles from failed fuel cladding into the canister interior, and ultimately, through a SCC.

The Tibetan Plateau space-based tropospheric aerosol climatology: 2007–2020

Abstract. A comprehensive and robust dataset of tropospheric aerosol properties is important for understanding the effects of aerosol–radiation feedback on the climate system and reducing the uncertainties of climate models. The “Third Pole” of Earth (Tibetan Plateau, TP) is highly challenging for obtaining long-term in situ aerosol data due to its harsh environmental conditions. Here, we provide the more reliable new vertical aerosol index (AI) parameter from the spaceborne-based lidar CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) on board CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) for daytime and nighttime to investigate the aerosol's climatology over the TP region during 2007–2020. The calculated vertical AI was derived from the aerosol extinction coefficient (EC), which was rigorously quality-checked and validated for passive satellite sensors (MODIS) and ground-based lidar measurements. Generally, our results demonstrated that there was agreement of the AI dataset with the CALIOP and ground-based lidar. In addition, the results showed that, after removing the low-reliability aerosol target signal, the optimized data can obtain the aerosol characteristics with higher reliability. The data also reveal the patterns and concentrations of high-altitude vertical structure characteristics of the tropospheric aerosol over the TP. They will also help to update and make up the observational aerosol data in the TP. We encourage climate modelling groups to consider new analyses of the AI vertical patterns, comparing the more accurate datasets, with the potential to increase our understanding of the aerosol–cloud interaction (ACI) and aerosol–radiation interaction (ARI) and their climate effects. Data described in this work are available at https://doi.org/10.11888/Atmos.tpdc.300614 (Huang, 2023).

Chemical characterization of atmospheric aerosols at a high-altitude mountain site: a study of source apportionment

Abstract. The study of aerosols in high mountain regions is essential because particulate matter can play a role in altering the energy balance of high mountain regions, and aerosols can accelerate glacier melting in high mountain areas by darkening the ice surface, reducing its reflectivity (albedo). Studying aerosols in high mountain areas provides insights into long-range transport of pollutants, atmospheric dynamics, and climate change impacts. These regions can serve as valuable observatories for studying atmospheric processes. The main aim of this paper is to define the main sources of aerosols over an entire year of sampling at the Col Margherita Atmospheric Observatory (MRG; 46°22′0.059′′ N, 11°47′30.911′′ E; 2543 m a.s.l.), a high-altitude background site in the eastern Italian Alps. Here, we discuss the potential origins of more than 100 chemical markers (major ions, water-soluble organic compounds, trace elements, and rare earth elements) using different approaches. Some diagnostic ratios were applied, but source apportionment using positive matrix factorization (PMF) was used to define the main inputs of PM10 collected at this high-altitude site, resulting in the identification of four factors: (1) Saharan dust events, (2) long-range marine/anthropogenic influence, (3) biogenic sources, and (4) biomass-burning and anthropogenic emissions. It can be inferred that, despite the distant location of the Col Margherita site, both regional pollution and long-range anthropogenic pollution have discernible effects on this area.

Chemical characterization and sources of background aerosols in the eastern Mediterranean

Measurements of the composition of the gas and particulate phases were conducted from May 9 to June 4 of 2016 at the Finokalia (Greece) remote coastal site in the eastern Mediterranean, continuing the effort to track long term changes of the atmospheric chemical composition in the area. Finokalia is influenced by air masses arriving in the site from regional sources in Europe, Africa, and other locations. In this study, a series of instruments and analysis techniques were used for the first time at the Finokalia site to characterize the composition of the organic aerosol (OA). The PM1 was composed of ammonium sulfate/bisulfate (60%), followed by organics (35%) and black carbon (BC) (4%). The OA was highly oxidized with an average oxygen-to-carbon (O:C) ratio of 0.81. Source apportionment of high-resolution organic aerosol mass spectra via positive matrix factorization (PMF) identified four factors: less oxidized oxygenated organic aerosol (LO-OOA), more oxidized oxygenated organic aerosol (MO-OOA), marine-related oxygenated organic aerosol (marine-OOA) and hydrocarbon-like organic aerosol (HOA). The LO-OOA (O:C = 0.92) was the dominant factor for most of the campaign (51% of the PM1 OA), while the MO-OOA (O:C = 1.1) was responsible for 11% of the OA. The marine-OOA factor was also highly oxidized (O:C = 1.03), contributing on average 24% to the total OA and was found to be well correlated with sulfate (R2 = 0.83). The anthropogenic HOA factor (O:C = 0.36) was related to activities in the island of Crete. Its mass spectrum was quite similar (R2 = 0.86–0.95) to those of other HOA factors in the literature and its average concentration was 0.2 μg m−3 (14% of OA). High molecular weight compounds were found, suggesting the presence of oligomers in agreement with the presence of a highly oxidized quenching agent. Aromatic VOCs, like benzene, toluene, and xylenes were on average 0.17, 0.66 and 0.36 ppb, respectively with toluene concentrations indicating the presence of a local source despite the remote nature of the site. New particle formation (NPF) was observed during 26% of the days. The air masses during NPF events passed over the island of Crete and the Balkans and were characterized by a low condensation sink (5.9 ± 2.2 10−3 s−1). Nucleation mode particle concentrations during NPF days had an additional evening peak between 17:00 and 22:00, which was accompanied by an HOA peak implying the influence of a source of sub-25 nm particles in the extended area. These findings show that even a relatively remote site like Finokalia is occasionally affected by sources located tens of kilometers away, something that should be taken into account in the interpretation of past and future measurements in this location.

Vertical Characteristics of HCHO and NO2 in Suburban Shanghai: Understanding of Ozone formation sensitivity via Secondary HCHO

Abstract Since ozone (O3) pollution in China is on the rise, vertical distribution of nitrogen dioxide (NO2) and formaldehyde (HCHO) and their role towards O3 formation are critical towards designing O3 control strategies. Seasonal characteristics of aerosols, HCHO and NO2 were investigated over suburban Shanghai using Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) from June 2020 to May 2021. For HCHO, the highest average vertical mixing ratios (VMRs) were observed for summer (0.775 ppb), followed by autumn (0.719 ppb), spring (0.718 ppb) and winter (0.672 ppb) at ground level. Seasonal trends in NO2 VMRs were observed to be opposite to that of HCHO with peak values occurring during winter (2.212 ppb) at the ground level followed by autumn (1.881 ppb), spring (1.415 ppb) and summer (1.124 ppb). In vertical, aerosols depicted a Gaussian shape with a higher values between 0.2 - 0.5 km. An exponential decay in NO2 VMRs is observed from 0.0 km to 3.0 km while the integral component of HCHO was found to be concentrated up to 2.0 km particularly during summer months. The vertical distribution of NO2 in different seasons mainly appeared below 0.5 km, while that of HCHO appeared within the range of 0.2-1.0 km. Both aerosols and NO2 tend to be higher during haze days compared to non-haze days while HCHO was found to be higher during clear days owing to high photochemical activity on a clear day. Based on the ratio of HCHO to NO2 (RFN), this study attempted to quantify the vertical characteristics of O3 sensitivity for different seasons. The results indicated that the O3 sensitivity was VOC-limited both at lower (generally, 0.0 - 0.6 km) and higher heights (1.8 - 3.0 km) while some transition limited scenarios were found at middle height (0.7 – 1.7 km) particularly during daytime. The results depicted that secondary HCHO is a crucial factor controlling on O3 sensitivity over Shanghai where enhanced ratio of VOC limited regime was observed with secondary HCHO for all the seasons.

Microfluidics produced ATRA-loaded PLGA NPs reduced tuberculosis burden in alveolar epithelial cells and enabled high delivered dose under simulated human breathing pattern in 3D printed head models

Tuberculosis, caused by Mycobacterium tuberculosis (Mtb), is second only to COVID-19 as the top infectious disease killer worldwide. Multi-drug resistant TB (MDR-TB) may arise because of poor patient adherence to medications due to lengthy treatment duration and side effects. Delivering novel host directed therapies (HDT), like all trans retinoic acid (ATRA) may help to improve drug regimens and reduce the incidence of MDR-TB. Local delivery of ATRA to the site of infection leads to higher bioavailability and reduced systemic side effects. ATRA is poorly soluble in water and has a short half-life in plasma. Therefore, it requires a formulation step before it can be administered in vivo. ATRA loaded PLGA nanoparticles suitable for nebulization were manufactured and optimized using a scalable nanomanufacturing microfluidics (MF) mixing approach (MF-ATRA-PLGA NPs). MF-ATRA-PLGA NPs demonstrated a dose dependent inhibition of Mtb growth in TB-infected A549 alveolar epithelial cell model while preserving cell viability. The MF-ATRA-PLGA NPs were nebulized with the Aerogen Solo vibrating mesh nebulizer, with aerosol droplet size characterized using laser diffraction and the estimated delivered dose was determined. The volume median diameter (VMD) of the MF-ATRA-PLGA NPs was 3.00 ± 0.18 μm. The inhaled dose delivered in adult and paediatric 3D printed head models under a simulated normal adult and paediatric breathing pattern was found to be 47.05 ± 3 % and 20.15 ± 3.46 % respectively. These aerosol characteristics of MF-ATRA-PLGA NPs supports its suitability for delivery to the lungs via inhalation. The data generated on the efficacy of an inhalable, scalable and regulatory friendly ATRA-PLGA NPs formulation provides a foundation on which further pre-clinical testing can be built. Overall, the results of this project are promising for future research into ATRA loaded NPs formulations as inhaled host directed therapies for TB.

Improving Dust Aerosol Optical Depth (DAOD) Retrieval from the GEOKOMPSAT-2A (GK-2A) Satellite for Daytime and Nighttime Monitoring.

The Advanced Meteorological Image (AMI) onboard GEOKOMPSAT 2A (GK-2A) enables the retrieval of dust aerosol optical depth (DAOD) from geostationary satellites using infrared (IR) channels. IR observations allow the retrieval of DAOD and the dust layer altitude (24 h) over surface properties, particularly over deserts. In this study, dust events in northeast Asia from 2020 to 2021 were investigated using five GK-2A thermal IR bands (8.7, 10.5, 11.4, 12.3, and 13.3 μm). For the dust cloud, the brightness temperature differences (BTDs) of 10.5 and 12.3 μm were consistently negative, while the BTD of 8.7 and 10.5 μm varied based on the dust intensity. This study exploited these optical properties to develop a physical approach for DAOD lookup tables (LUTs) using IR channels to retrieve the DAOD. To this end, the characteristics of thermal radiation transfer were simulated using the forward model; dust aerosols were explained by BTD (10.5, 12.3 μm)-an intrinsic characteristic of dust aerosol. The DAOD and dust properties were gained from a brightness temperature (BT) of 10.5 μm and BTD of 10.5, 12.3 μm. Additionally, the cumulative distribution function (CDF) was employed to strengthen the continuity of 24-h DAOD. The CDF was applied to the algorithm by calculating the conversion value coefficient for the DAOD error correction of the IR, with daytime visible aerosol optical depth as the true value. The results show that the DAOD product can be successfully applied during the daytime and nighttime to continuously monitor the flow of yellow dust from the GK-2A satellite in northeast Asia. In particular, the validation results for IR DAOD were similar to the active satellite product (CALIPSO/CALIOP) results, which exhibited a tendency similar to that for IR DAOD at night.

Comparative Study of Aerosol Optical Properties along a Megacity

Interest in the study and characterization of aerosols has been growing given its multiple connections with air quality and climate. However, the limited ground-based stations for measurements in many countries are not enough to completely study a big city or a region. Low-cost technology arises as a viable alternative to improve the spatial resolution of measurements. This study aims to demonstrate that the properties of aerosols may change within a megacity and that is advisable to segment measurements according to their characteristics. We measured the optical properties of aerosols in the outskirts of Buenos Aires and compared the data obtained with AERONET data from the city center. This is the first study of its kind in the region. The comparison of concentration, sizes, and types of aerosols shows differences between the sites regardless of the background levels that they share regionally. While the city center has a strong influence from traffic and sea particles and levels of pollution typical of a dense city, the outskirts present several aerosol sources and characteristics of a semi-rural site with a moderate influence of anthropogenic sources.

Investigation of Light-Scattering Properties of Non-Spherical Sea Salt Aerosol Particles at Varying Levels of Relative Humidity

In the marine environment, sea salt aerosol particles transition from cubic or rectangular shapes when dry to various non-spherical shapes like ellipsoids and cylinders under different humidities. The complex humidity conditions and particle morphologies pose challenges to simulating the optical scattering properties of non-spherical sea salt aerosols. This study, addressing real environmental scenarios, employs the randomly oriented T-matrix computational method to calculate the optical scattering and polarization characteristics of sea salt aerosols at a wavelength of 1.06 μm under three relative humidity conditions (50%, 80%, and 95%) and three particle morphologies (spheroid, circular cylinder, and Chebyshev particle shapes). The results show the following: (1) In terms of optical scattering properties, the greater the non-sphericity of particles under the same humidity conditions, the larger the deviation between non-spherical and spherical models. For spheroid and circular cylinder sea salt aerosols, the error in the extinction efficiency factor mainly lies within 10–30%, reaching up to 120%; the error in the asymmetry factor is primarily between 3 and 25%, with a maximum of 75%, and the error in the forward-scattering phase function is mainly within 10–60%, reaching up to 180%. Chebyshev particle-shaped sea salt aerosols exhibit smaller deviations in optical scattering properties compared to equivalent spherical models, generally within the 5–25% range. Under different humidity conditions, the scattering characteristic parameters of sea salt aerosol particles for various non-spherical models show a positive correlation with relative humidity. When relative humidity is below 70%, the optical scattering properties of differently shaped sea salt aerosols are less affected by relative humidity. Above 70% relative humidity, the optical scattering properties of sea salt aerosols of different shapes become more sensitive to changes in relative humidity. (2) Regarding polarization properties, the greater the humidity, the more significant the impact on polarization properties, and as humidity increases, sea salt aerosols with higher non-sphericity exhibit more complex changes in polarization characteristics. The differences in shapes of non-spherical models mainly affect the numerical values of polarization properties. Under the same humidity conditions, spheroid polarization characteristics are significantly different from other models. In terms of depolarization ratio for aerosols, circular cylinder sea salt aerosols show the highest depolarization ratio at various relative humidities, followed by spheroid, with Chebyshev-shaped having the least. The effect of relative humidity on the depolarization ratio varies with the scattering angle. The higher the relative humidity, the more complex the variation in the depolarization ratio with scattering angle, with more pronounced oscillations in the curve, and the less non-spherical the shape, the more intense the oscillations in the depolarization ratio curve due to humidity. In conclusion, this study calculated the optical scattering and polarization properties of sea salt aerosol particles under different relative humidities and shapes, which is of significant importance for applications like 1.06 μm laser engineering and atmospheric radiation transmission in actual marine scenarios.

Characterization of airborne dust emissions from three types of crushed multi-walled carbon nanotube-enhanced concretes

Dispersing Multi-Walled Carbon Nanotubes (MWCNTs) into concrete at low (<1 wt% in cement) concentrations may improve concrete performance and properties and provide enhanced functionalities. When MWCNT-enhanced concrete is fragmented during remodelling or demolition, the stiff, fibrous and carcinogenic MWCNTs will, however, also be part of the respirable particulate matter released in the process. Consequently, systematic aerosolizing of crushed MWCNT-enhanced concretes in a controlled environment and measuring the properties of this aerosol can give valuable insights into the characteristics of the emissions such as concentrations, size range and morphology. These properties impact to which extent the emissions can be inhaled as well as where they are expected to deposit in the lung, which is critical to assess whether these materials might constitute a future health risk for construction and demolition workers. In this work, the impact from MWCNTs on aerosol characteristics was assessed for samples of three concrete types with various amounts of MWCNT, using a novel methodology based on the continuous drop method. MWCNT-enhanced concretes were crushed, aerosolized and the emitted particles were characterized with online and offline techniques. For light-weight porous concrete, the addition of MWCNT significantly reduced the respirable mass fraction (RESP) and particle number concentrations (PNC) across all size ranges (7 nm – 20 μm), indicating that MWCNTs dampened the fragmentation process by possibly reinforcing the microstructure of brittle concrete. For normal concrete, the opposite could be seen, where MWCNTs resulted in drastic increases in RESP and PNC, suggesting that the MWCNTs may be acting as defects in the concrete matrix, thus enhancing the fragmentation process. For the high strength concrete, the fragmentation decreased at the lowest MWCNT concentration, but increased again for the highest MWCNT concentration. All tested concrete types emitted <100 nm particles, regardless of CNT content. SEM imaging displayed CNTs protruding from concrete fragments, but no free fibres were detected.

Optical characterization of native aerosols from e-cigarettes in localized volumes.

Measuring the size distribution of aerosols typically requires processing a sample, specifically to adjust the particle concentration to an adequate level. Unfortunately, this manipulation can significantly alter the native composition of some aerosols, which can lead to unreliable or even unusable measurements. We demonstrate that coherence-gated dynamic light scattering is suitable to measure the size distribution of native aerosols without the need for sample processing. Another novel aspect of the present work is the first demonstration of these type of localized light-scattering-based measurements in aerial media. Measuring the size distribution reliably in optically dense aerosols is possible thanks to the interferometric amplification of single scattering in an optically isolated, picolitre-sized coherence volume. We carried out proof-of-concept experiments in aerosols from electronic cigarettes, which poses a challenge mainly due to their high concentration, volatility, and hygroscopicity. We generated aerosols using two common moisturizers, propylene glycol and glycerol, and measured their particle size distribution as a function of the burning power. The aerosols generated in the presence of glycerol are more polydisperse and have larger particles with increasing burning power. This unique characterization of native aerosols can provide valuable information for dosimetry and hosting sites in the respiratory system.

Characterization and apportionment of carbonaceous aerosol emission factors from light-duty and heavy-duty vehicle fleets in Maharashtra, India

This study aims to investigate the characteristics of carbonaceous aerosols and estimate emission factor (EF) based on roadway tunnel measurements, from two distinct vehicular fleets: an all light-duty vehicle (LDV) fleet, and a mixed fleet of 80% LDV and 20% heavy-duty vehicle (HDV). Carbonaceous content (organic carbon: OC and elemental carbon: EC) in total fine particles (PM2.5) accounted for 41% ± 6.8% in LDV fleet and 48% ± 7.2% in mixed fleet. While higher volatile OC dominated in the LDV fleet emissions, in mixed fleet, lower volatile OC and EC emissions dominated due to the presence of higher HDV and super-emitter (SE) fractions which led to significantly higher optically active absorbing aerosols. Reconstructed HDV fleet EF was higher than LDV fleet by 36 times (PM2.5), 19 times (OC) and 51 times (EC). Our findings emphasize the significance of implementing vehicle inspection and maintenance programs, coupled with decarbonization of HDVs to mitigate on-road vehicular emissions in India.

Analysis of Aerosol Types and Vertical Distribution in Seven Typical Cities in East Asia

Identifying the types and vertical distribution of aerosols plays a significant role in evaluating the influence of aerosols on the climate system. Based on the aerosol optical properties obtained from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), this study analyzed the long-term aerosol characteristics of seven cities in East Asia (Ulaanbaatar, Beijing, Lanzhou, Shanghai, Lhasa, Hong Kong, and Bangkok) from 2007 to 2021, including the spatiotemporal variations of aerosol optical depth (AOD), the vertical stratification characteristics of aerosols, and the main aerosol subtype. The results showed that, except for Lhasa, the AOD values of all cities exhibited a trend of initially increasing and then decreasing over the years. Except for Shanghai, the high values of AOD in the other cities occurred in the spring and summer seasons, while the low values occurred in the autumn and winter seasons. In all four seasons, the AOD contribution within the 1–3 km range accounted for more than 50% of the total. In the autumn and winter seasons, this proportion reached over 80%. The main types of aerosols and their contributions varied at different altitudes. Overall, dust, polluted continental/smoke, polluted dust, and elevated smoke dominated in all aerosol layers across each city. On the other hand, clean marine, clean continental, and dusty marine had very small proportions, accounting for less than 5% of all the cities’ aerosol layers.

Characteristics of Aerosols and Clouds and Their Role in Earth’s Energy Budget

Abstract Clouds and aerosols provide the greatest uncertainty in estimating and interpreting Earth’s energy budget. This study not only focuses on surface brightening/dimming, but also explores Earth’s energy balance. The validation results of the CERES-SYN, ISCCP-FH, and GEWEX-SRB datasets with Baseline Surface Radiation Network (BSRN), Surface Radiation Budget Network (SURFRAD), and CMA observations show that CERES data have the highest accuracy and the longest temporal coverage. The role of clouds and aerosols in Earth’s energy budget was explained using CERES and MERRA-2 products. The results show that Earth’s energy increases at a rate of 0.63 W m−2 decade−1 in 2000–21. The global surface brightens at a rate of 0.57 W m−2 decade−1, with surface energy decreasing at a rate of 0.19 W m−2 decade−1. Brightening was found over Australia, central Asia, and southern Africa, mainly associated with cloud reduction, with aerosol emissions reductions contributing to the East Asian surface brightening. The surface brightening in South America and Southeast Asia is also due to the reduction of clouds. The increase of aerosols in South Asia is the main factor for its surface dimming, while we infer that the climatic effect from the increase of black carbon (BC) aerosols in South Asia is the inducing factor for the dimming in southern China. The surface darkening in West Asia is the result of the combined effect of clouds and aerosols, while in northern Africa it may be related to the increase of clouds caused by the decrease of dust aerosols. Surface energy increases only in Southeast Asia, South America, and Europe. Significance Statement Clouds and aerosols provide the greatest uncertainty in estimating and interpreting Earth’s changing energy budget. Moreover, the relative importance of clouds and aerosols is variable, depending on the regions and time scales of studies. This study shows that the energy inflow to the Earth system is greater than the energy outflow in 2000–21, with radiation on Earth increasing at a rate of 0.63 W m−2 decade−1 with the surface energy decreases at a rate of 0.19 W m−2 decade−1. Brightening was found over Southeast Asia, South America, Australia, and southern Africa, with the areas of surface darkening occurring mainly in Asia and northern Africa.

Insights into the seasonal characteristics of single particle aerosols in Chengdu based on SPAMS

To investigate the seasonal characteristics in air pollution in Chengdu, a single particle aerosol mass spectrometry was used to continuously observe atmospheric fine particulate matter during one-month periods in summer and winter, respectively. The results showed that, apart from O3, the concentrations of other pollutants (CO, NO2, SO2, PM2.5 and PM10) were significantly higher in winter than in summer. All single particle aerosols were divided into seven categories: biomass burning (BB), coal combustion (CC), Dust, vehicle emission (VE), K mixed with nitrate (K-NO3), K mixed with sulfate and nitrate (K-SN), and K mixed with sulfate (K-SO4) particles. The highest contributions in both seasons were VE particles (24%). The higher contributions of K-SO4 (16%) and K-NO3 (10%) particles occurred in summer and winter, respectively, as a result of their different formation mechanisms. S-containing (K-SO4 and K-SN), VE, and BB particles caused the evolution of pollution in both seasons, and they can be considered as targets for future pollution reduction. The mixing of primary sources particles (VE, Dust, CC, and BB) with secondary components was stronger in winter than in summer. In summer, as pollution worsens, the mixing of primary sources particles with 62 [NO3]− weakened, but the mixing with 97 [HSO4]− increased. However, in winter, the mixing state of particles did not exhibit an obvious evolution rules. The potential source areas in summer were mainly distributed in the southern region of Sichuan, while in winter, besides the southern region, the contribution of the western region cannot be ignored.

HETEAC-Flex: an optimal estimation method for aerosol typing based on lidar-derived intensive optical properties

Abstract. This study introduces a novel methodology for the characterization of atmospheric aerosol based on lidar-derived intensive optical properties. The proposed aerosol-typing scheme is based on the optimal estimation method (OEM) and allows the identification of up to four different aerosol components of an aerosol mixture, as well as the quantification of their contribution to the aerosol mixture in terms of relative volume. The four aerosol components considered in this typing scheme are associated with the most commonly observed aerosol particles in nature and are assumed to be physically separated from each other and, therefore, can create external mixtures. Two components represent absorbing and less-absorbing fine-mode particles, and the other two components represent spherical and non-spherical coarse-mode particles. These components reflect adequately the most frequently observed aerosol types in the atmosphere: combustion- and pollution-related aerosol, sea salt, and desert dust, respectively. In addition, to consolidate the calibration and validation efforts for the upcoming EarthCARE mission, the typing scheme proposed here is in accordance with the Hybrid End-To-End Aerosol Classification (HETEAC) model of EarthCARE. The lidar-derived optical parameters used in this typing scheme are the lidar ratio and the particle linear depolarization ratio at two distinct wavelengths (355 and 532 nm), the backscatter-related color ratio for the wavelength pair of 532/1064 nm and the extinction-related Ångström exponent for the wavelength pair of 355/532 nm. These intensive optical properties can be combined in different ways, making the methodology flexible, thus allowing its application to lidar systems with different configurations (e.g., single wavelength or multiwavelength, Raman, high spectral resolution). The typing scheme was therefore named HETEAC-Flex due to its compatibility with EarthCARE's HETEAC and its methodological flexibility. The functionality of the typing scheme is demonstrated by its application to three case studies based on layer-averaged optical properties.

Aerosol characterization and peculiarities of source apportionment in Moscow, the largest and northernmost European megacity

High population and a wide range of activities in a megacity lead to large-scale ecological consequences which require the assessment with respect to distinct characteristics of climate, location, fuel consumption, and emission sources. In-depth study of aerosol characteristics was carried out in Moscow, the largest megacity in Europe, during the cold period (autumn and winter) and in spring. PM10 chemical speciation based on carbonaceous matter, water-soluble ions, and elements was carried out to reconstruct the PM mass and evaluate the primary and secondary aerosol contribution. For the whole study period organic matter, mineral dust, and secondary inorganic/organic accounted for 34, 24, and 16 % of PM10 mass, respectively. PM10, OC, and EC approached a maximum in spring and decreased in winter. Mineral dust seasonal fraction increased from spring (17 %) to autumn (32 %), and then decreased in winter (22 %). Secondary inorganic aerosols (SIA) in opposite showed the maximum 27 % in winter. K+ marked the residential biomass burning in the region surrounding a megacity in spring and autumn, agriculture fires in spring. In winter primary aerosol contribution dropped down 56 % while secondary approached practically equal 44 %. Source factors with the relative contributions are quantified, namely city dust (26 %), traffic (23 %), industrial (20 %), biomass burning (12 %), secondary (12 %), and de-icing salt (7 %); they were significantly varying between the cold heating period and springtime. The relevance of sources to meteorological parameters and mass transportation is investigated by using both bivariate polar plots and Lagrangian integrated trajectory (HYSPLIT) model. Trajectory clustering demonstrates regional sources being crucial contributors to PM10 pollution. Aerosol speciation and source apportion factors identify the differences of the Moscow urban background among large European and Asian cities due to northern climate conditions, fast construction, long-range transport from industrial-developing area surrounding a city, regional biomass burning preferably in spring and autumn, and winter road management.

Positive matrix factorization of seasonally resolved organic aerosol at three different central European background sites based on nuclear magnetic resonance Aerosolomics data

Concentration data derived from 1H NMR analysis of the water-soluble organic compounds from fine aerosol (PM2.5) at three Central European background stations, Košetice, Frýdlant (both in the Czech Republic), and Melpitz (Germany), were used for detailed source apportionment analysis. Two winter and two summer episodes (year 2021) with higher organic concentrations and similar wind directions were selected for NMR analyses. The concentration profiles of 61 water-soluble organic compounds were determined by NMR Aerosolomics and a principal component analysis (PCA) was performed on this dataset. Based on the PCA results, 23 compounds were selected for positive matrix factorization (PMF) analysis in order to identify dominant aerosol sources at rural background sites in Central Europe. Both the PCA and the subsequent PMF analyses clearly distinguished the characteristics of winter and summer aerosol particles.In summer, four factors were identified from PMF and were associated with biogenic aerosol (61–78 %), background aerosol (9–15 %), industrial biomass combustion (7–13 %), and residential heating (5–13 %). In winter, only 3 factors were identified - industrial biomass combustion (33–49 %), residential heating (37–45 %) and a background aerosol (8–30 %). The main difference was observed in the winter season with a stronger contribution of emissions from industrial biomass burning at the Czech stations Košetice and Frýdlant (47–49 %) compared to the Melpitz station (33 %). However, in general, there were negligible differences in identified sources between stations in the given seasons, indicating a certain homogeneity in PM2.5 composition within Central Europe at least during the sampling periods.