Ambient Aerosol Research Articles

Positive Feedback between Partitioning of Carbonyl Compounds and Particulate Sulfur Formation during Haze Episodes.

Carbonyl compounds are important precursors of aqueous aerosols in the atmosphere, while their gas-particle partitioning behaviors and roles in particulate sulfur formation are poorly understood. In this study, we investigate the partitioning of five carbonyl compounds (formaldehyde, acetaldehyde, acetone, glyoxal, and methylglyoxal) during haze episodes in Beijing, China. On haze days, the values of field-derived effective Henry's law coefficients (KHf) on aerosols for these carbonyl compounds are 106-108 M atm-1, which are significantly higher (102-104 times) than those in pure water. Sulfate is observed to have a pronounced "salting-in" effect on these carbonyl compounds, resulting in at least 1-order-of-magnitude increase in their particle-phase concentrations. Parameterization schemes for their partitioning in the ambient aerosols were provided and applied to the multiphase chemical box model (RACM2-CAPRAM). When incorporated into the field-derived parametrization, the model significantly increased hydroxymethanesulfonate (HMS) production by 50-fold compared to using the parameters obtained in pure water, increasing from 2.6 × 10-2 to 1.23 μg m-3 h-1. The formed HMS can facilitate sulfate formation in turn through further oxidation by OH radicals and enhance aerosol hygroscopicity. These findings indicate a positive feedback loop between the partitioning of carbonyl compounds and particulate sulfur formation during haze episodes, providing new insights for controlling particulate pollution and reducing SO2 levels in urban areas.

Predictions of the Optical Properties of Brown Carbon Aerosol by Machine Learning with Typical Chromophores.

The linkages between BrC optical properties and chemical composition remain inadequately understood, with quantified chromophores explaining less than 25% of ambient aerosol light absorption. This study characterized 38 typical chromophores in aerosols collected in Xi'an, with light absorption contributions to BrC ranging from 1.6 ± 0.3 to 5.8 ± 2.6% at 365 nm. Based on these quantified chromophores, an interpretable machine learning model and the Shapley Additive Explanation (SHAP) method were employed to explore the relationships between BrC optical properties and chemical composition. The model attained high accuracy with Pearson correlation coefficients (r) exceeding 0.93 for the absorption coefficient (Absλ) and surpassing 0.57 for mass absorption efficiency (MAEλ) of BrC. It explains more than 80% of the variance in Abs and over 50% in MAE, significantly improving the understanding of BrC light absorption. Polycyclic aromatic hydrocarbons (PAHs) and oxygenated PAHs (OPAHs) with four and five rings exhibit significant positive effects on Absλ, suggesting that similar unidentified chromophores may also notably impact BrC optical characteristics. The model based on chromophore mass concentrations further simplifies studying BrC optical characteristics. This study advances understanding of the relationship between BrC composition and optical properties and guides the investigation of unrecognized chromophores.

Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods

Abstract. Since most people, especially in developed countries, spend most of their time indoors, they are heavily exposed to indoor aerosols, which can potentially lead to adverse health effects. A major source of indoor aerosols are cooking activities, which release large quantities of particulate emissions (in terms of both number and mass), often with complex compositions. To investigate the characteristics of cooking emissions and what influences these emissions, we conducted a comprehensive study by cooking 19 dishes with different ingredients and cooking methods. The emissions were monitored in real time with several online instruments that measured both physical and chemical particle properties as well as trace gas concentrations. The same instrumentation was used to study the influence of cooking emissions on the ambient aerosol load at two German Christmas markets. In contrast to previous studies, which often focus on individual aspects or emission variables, this broad and coherent approach allows a comparison of the influence of different parameters (e.g., ingredients, cooking method, cooking temperature, cooking activities) on the emissions. We found an influence of cooking emissions on six variables: number concentration of smaller (particle diameter dp > 5 nm) and larger (dp > 250 nm) particles, particulate matter (PM: PM1, PM2.5, PM10), black carbon (BC), PAHs (polycyclic aromatic hydrocarbons), and organic aerosol mass concentration. In general, similar emission characteristics were observed for dishes with the same cooking method, mainly due to similar cooking temperature and use of oil. The temporal dynamics in the emissions of the aforementioned variables, as well as the sizes of the emitted particles, were mainly influenced by the cooking temperature and the activities during cooking. Emissions were quantified using emission factors, with the highest values for grilled dishes, 1 to 2 orders of magnitude lower for oil-based cooking (baking, stir-frying, deep-frying), and the lowest for boiled dishes. For the identification of cooking emissions with the Aerodyne aerosol mass spectrometer (AMS), and more generally for the identification of new AMS markers for individual organic aerosol types, we propose a new plot type that takes into account the mass spectral variability for individual aerosol types. Combining our results and those of previous studies for the quantification of cooking-related organic aerosols with the AMS, we recommend the use of relative ionization efficiency values higher than the default value for organics (RIEOrg = 1.4): 2.17 ± 0.48 for rapeseed-oil-based cooking and 5.16 ± 0.77 for soybean-oil-based cooking.

Winter haze amplification by aerosol hygroscopic growth over eastern Indo- Gangetic Plain

Frequent occurrences of widespread winter haze over Northern India largely appear to originate from exceedingly high concentrations of fine particulate matter from anthropogenic emissions. However, the underlying mechanisms driving winter haze in Northern India are not well understood. This study employed a synergy of satellite and reanalysis data from 2006 to 2021 to assess the role of hygroscopic growth of aerosol optical depth in winter haze over the eastern Indo-Gangetic Plain. A method has been developed to extract dry aerosol optical depth from ambient aerosol optical depth to elucidate the origin of winter haze. About 31% of severe haze episodes (aerosol optical depth > 0.85) occurring under ambient humidity conditions decrease to below 5% for dry conditions, indicating the critical role of particle hygroscopic growth. The change in radiative forcing at the top of the atmosphere due to hygroscopic growth is relatively small compared to that at the surface and in the atmosphere, indicating enhanced atmospheric warming. The ubiquitous winter haze over the eastern Indo-Gangetic Plain is exacerbated by hygroscopic growth under high anthropogenic aerosol emissions, further aggravated through aerosol-radiation feedback. These results will be valuable in devising haze forecasts, implementing effective mitigation policies, and representing aerosol hygroscopicity in climate models.

African dust: Occurrence, health consequences, and impacts on Texas

The drylands of North Africa (Sahara and Sahel) are the world’s largest sources of airborne dust. Clouds of African dust aerosols have been long known to be blown westwards across the Atlantic, and by the 1990s were recognized to be transported across and over Texas. African dust incursions in Texas typically happen several times per year in late spring and summer, manifesting as hazy skies overhead and increased ground-level concentrations of PM2.5 (particulate matter fine enough to be inhaled into the human lower respiratory tract). African dust exposure has many reported human health effects in Europe and the Caribbean, including increased all-cause mortality and increased respiratory and cardiovascular disease morbidity and mortality. In Texas, African dust’s greatest impacts occur in the Houston metropolitan area where it has been quantitatively shown to increase ambient aerosol concentrations. The potential of African dust increasing concentrations of inhalable particulate matter beyond regulatory limits is of concern. A sequence of investigations filtering particles from the air, measuring their concentrations, and subjecting them to elemental analysis documented far-transported African dust’s role in air quality in Houston and Galveston. African dust’s contributions to air pollution have been separated from those of local soils and industrial emissions, and Saharan-Sahelian dust has been indicated to sometimes constitute the majority of PM2.5 mass in Houston. While studies show the presence of inhalable metals and microorganisms including opportunistic pathogens during Saharan air incursions in Houston, the human health effects of African dust in Texas remain yet unspecified and merit further investigation. Keywords: aerosols; Africa, Northern; air pollution; dust; particulate matter; public health; Texas

Optical and Physico-chemical Characteristics of Ambient Aerosols Along Gangotri Glacier Valley in Western Himalaya, India

Optical and Physico-chemical Characteristics of Ambient Aerosols Along Gangotri Glacier Valley in Western Himalaya, India

Single-stage NBI sampler for PM1 mass and five-stage NBI-NMCI sampler for PM1 mass distribution measurements

In recent years, concerns about the health and environmental risks associated with PM1 particles have increased. However, existing PM1 sampling instruments remain to be improved mainly because their PM1 inlets have particle loading and bounce issues. To address these challenges, PM1 inlets based on the Non-Bouncing Impactor (NBI) technique were developed. These inlets employ vacuum oil-wetted glass fiber filter (GFF) substrates to eliminate particle bounce and incorporate a daily vacuum oil injection to prevent particle loading. The 16.7 L/min PM1 NBI, modified from the PM2.5 M-WINS design with a reduced diameter of the single nozzle, was designed to adapt readily with current standard sampling and monitoring systems. The cut-size (Dpa50) of 0.99 ± 0.02 μm was determined by considering the effects of Reynold number and the ratio of jet-to-plate distance and nozzle diameter. Field tests comparing the 16.7 L/min PM1 NBI sampler to the 9-stage NCTU Micro-orifice Cascade Impactor (NMCI9) revealed small sampling biases, with a mean difference of +0.26 ± 2.28 μg/m3 for PM1 measurements when silicone oil-coated aluminum foil (AF) and GFF-AF were used in the NMCI9. The NBI with the oil-wetted GFF substrate effectively removed particles larger than 1.0 μm, resulting in more accurate PM1 mass concentration measurements. Additionally, the development of a 5-stage NMCI with the 30 L/min PM1 NBI as the first stage enabled detailed measurement of PM1 mass distribution in two modes, which was challenging when measuring the entire mass distribution of ambient aerosols. The distribution of size-dependent water-soluble inorganic ions in PM1 showed dominance of SO42− and NH4+ in PM1 compared to PM2.5. In summary, the PM1 NBI enhances accuracy for long-term atmospheric sampling by addressing particle loading and bounce, making it a more reliable standard sampling instrument.

Effect of relative humidity on passive spore release from substrate surfaces

Fungal spores are abundant in ambient air and exposure to this type of bioaerosols are found to cause significant health and climatic effects. In this study, we investigated the influence of air relative humidity (RH) on the passive release of spores from solid substrates. Preliminary investigations into the effect of RH on fungal spore release indicated an increase in spore flux with reduced air RH. The change in spore emission flux occurred very quickly in response to a change in ambient RH. To verify the hypothesis of extremely rapid drying under lower RH, experiments were conducted using a quartz crystal microbalance with dissipation (QCM-D) to understand the timescales of spore moisture uptake and drying. The analysis of mass transfer of water to and from the spores indicated that the bulk of the transfer occurred within a minute of exposure to any RH. The effect of the ambient RH was explained using a mathematical model with the spotlight on the parameter, E, that represented the energy required to aerosolise one spore. This study demonstrates the application of QCM-D to study interaction between ambient aerosol particles and various vapor phase and gas phase environments. The study enhances the overall understanding and capability to characterise passive fungal spore release under varying humidity conditions in the natural environment.

Air pollution from unconventional oil and gas development in the Eagle Ford Shale

Unconventional oil and gas development (UOGD) has experienced substantial growth in recent years with currently unconstrained impacts on air quality. In this work, we describe ambient aerosol and gas-phase measurements during spring 2021 to examine air quality in the Eagle Ford Shale (EFS), a region in southeast Texas with thousands of UOGD wells. NOx, O3, H2S, PM1, and several VOCs were measured at concentrations above expected levels for non-urban regions. Hydrocarbon measurements from gas chromatography (GC) and proton transfer reaction (PTR) mass spectrometry show periodic high concentrations of variable compositions consisting of both saturated and unsaturated (polycyclic and/or aromatic) hydrocarbons, including larger (C > 10) unsaturated hydrocarbons that are often not quantified by GC measurements but are still present at substantial concentrations and relevant for air quality. Hydrocarbon VOCs are expected pollutants from anthropogenic activity and, based on ratios of i-pentane to n-pentane, xylene to benzene, and toluene to benzene, measured VOC ratios were characteristic of UOGD activity. Wind data and back-trajectory analyses show that air predominantly arrived from the S/SE, consistent with UOGD sources as well as shipping emissions from the Gulf of Mexico impacting air quality in the EFS. Analysis of diurnal trends at the site show hydrocarbon and NOx accumulation overnight and highlight diurnal differences in oxidative conditions, with important implications for both SOA and O3 formation. UOGD emissions impact the air quality in Karnes City and more broadly the EFS as well as the nearby urban area of San Antonio, which struggles to meet national air quality standards set by the Environmental Protection Agency.

International airport emissions and their impact on local air quality: chemical speciation of ambient aerosols at Madrid–Barajas Airport during the AVIATOR campaign

Abstract. Madrid–Barajas Airport (MAD) is the fourth-busiest airport in Europe. The aerosol chemical composition and the concentrations of other key pollutants were measured at the airport perimeter during October 2021 to assess the impact of airport emissions on local air quality. A high-fidelity ambient instrumentation system was deployed at Madrid–Barajas Airport to measure the following: concentrations of organic aerosols (with their composition), black carbon (eBC), carbon dioxide (CO2), carbon monoxide (CO), nitrogen dioxide (NOx), sulfur dioxide (SO2), particulate matter (PM2.5, PM10), total hydrocarbon (THC), and total particle number. The average concentrations of eBC, NOx, SO2, PM2.5, PM10, CO, and THC at the airport for the entire campaign were 1.07 µg m−3, 22.7 µg m−3, 4.10 µg m−3, 9.35 µg m−3, 16.43 µg m−3, 0.23 mg m−3, and 2.30 mg m−3, respectively. The source apportionment analysis of the non-refractory organic aerosol (OA) using positive matrix factorisation (PMF) allowed us to discriminate between different sources of pollution, namely less oxidised oxygenated organic aerosol (LO-OOA), alkane organic aerosol (AlkOA), and more oxidised oxygenated organic aerosol (MO-OOA). The results showed that LO-OOA and MO-OOA account for more than 80 % of the total organic particle mass measured near the runway. Trace gases correlate better with the AlkOA factor than LO-OOA and MO-OOA, indicating that AlkOA is mainly related to primary combustion emissions. Bivariate polar plots were used for pollutant source identification. Significantly higher concentrations of the obtained factors were observed at low wind speeds (<3 m s−1) from the southwest, where two of the runways and all terminals are located. Higher SO2/NOx and CO/eBC ratios were observed when the winds originated from the northeast, where the two northern runways are located. These elevated ratios are attributed to the aircraft activity being the major pollutant source in the northeast area.

Photolytic Degradation of Water‐Soluble Organic Carbon in Snowmelts: Changes in Molecular Characteristics, Brown Carbon Chromophores, and Radiative Effects

AbstractWater‐soluble organic carbon (WSOC) deposited in ambient snowpack play key roles in regional carbon cycle and surface energy budget, but the impacts of photo‐induced processes on its optical and chemical properties are poorly understood yet. In this study, melted samples of the seasonal snow collected from northern Xinjiang, northwestern China, were exposed to ultraviolet (UV) radiation to investigate the photolytic transformations of WSOC. Molecular characteristics and chemical composition of WSOC and its brown carbon (BrC) constituents were investigated using high‐performance liquid chromatography interfaced with a photodiode array detector and a high‐resolution mass spectrometer. Upon illumination, formation of nitrogen‐ and sulfur‐containing species with high molecular weight was observed in snow samples influenced by soil‐ and plant‐derived organics. In contrast, the representative sample collected from remote region showed the lowest molecular diversity and photolytic reactivity among all samples, in which no identified BrC chromophores decomposed upon illumination. Approximately 65% of chromophores in urban samples endured UV irradiation. However, most of BrC composed of phenolic/lignin‐derived compounds and flavonoids disappeared in the illuminated samples containing WSOC from soil‐ and plant‐related sources. Effects of the photochemical degradation of WSOC on the potential modulation of snow albedo were estimated. Apparent half‐lives of WSOC estimated as albedo reduction in 300–400 nm indicated 0.1–0.4 atmospheric equivalent days, which are shorter than typical photolysis half‐lives of ambient biomass smoke aerosol. This study provides new insights into the roles of WSOC in snow photochemistry and snow surface energy balance.

Quantifying New Sources of Ambient Organic Aerosol and Their Roles in Particle Growth Using Oxygenated Organic Molecule (OOM) Tracers

Quantifying New Sources of Ambient Organic Aerosol and Their Roles in Particle Growth Using Oxygenated Organic Molecule (OOM) Tracers

Evidence of Surface-Tension Lowering of Atmospheric Aerosols by Organics from Field Observations in an Urban Atmosphere: Relation to Particle Size and Chemical Composition.

Surface-active organics lower the aerosol surface tension (σs/a), leading to enhanced cloud condensation nuclei (CCN) activity and potentially exerting impacts on the climate. Quantification of σs/a is mainly limited to laboratory or modeling work for particles with selected sizes and known chemical compositions. Inferred values from ambient aerosol populations are deficient. In this study, we propose a new method to derive σs/a by combining field measurements made at an urban site in northern China with the κ-Köhler theory. The results present new evidence that organics remarkably lower the surface tension of aerosols in a polluted atmosphere. Particles sized around 40 nm have an averaged σs/a of 53.8 mN m-1, while particles sized up to 100 nm show σs/a values approaching that of pure water. The dependence curve of σs/a with the organic mass resembles the behavior of dicarboxylic acids, suggesting their critical role in reducing the surface tension. The study further reveals that neglecting the σs/a lowering effect would result in lowered ultrafine CCN (diameter <100 nm) concentrations by 6.8-42.1% at a typical range of supersaturations in clouds, demonstrating the significant impact of surface tension on the CCN concentrations of urban aerosols.

Physicochemical metamorphosis of re-aerosolized urban PM2.5

The toxicity of particulate matter (PM) is dependent on particle physical and chemical properties and is commonly studied using in vivo and in vitro approaches. PM to be used for in vivo and in vitro studies is often collected on filters and then extracted from the filter surface using a solvent. During extraction and further PM sample handling, particle properties change, but this is often neglected in toxicology studies, with possible implications for health effect assessment. To address the current lack of knowledge and investigate changes in particle properties further, ambient PM with diameter less than 2.5 μm (PM2.5) was collected on filters at an urban site and extracted using a standard methanol protocol. After extraction, the PM was dried, dispersed in water and subsequently nebulized. The resulting aerosol properties were then compared to those of the ambient PM2.5. The number size distribution for the nebulized aerosol resembled the ambient in terms of the main mode diameter, and >90 % of particle mass in the nebulized size distribution was still in the PM2.5 range. Black carbon made up a similar fraction of PM mass in nebulized as in ambient aerosol. The sulfate content in the nebulized aerosol seemed depleted and the chemical composition of the organic fraction was altered, but it remains unclear to what extent other non-refractory components were affected by the extraction process. Trace elements were not distributed equally across size fractions, neither in ambient nor nebulized PM. Change in chemical form was studied for zinc, copper and iron. The form did not appear to be different between the ambient and nebulized PM for iron and copper, but seemed altered for zinc. Although many of the studied properties were reasonably well preserved, it is clear that the PM2.5 collection and re-aerosolization process affects particles, and thus potentially also their health effects. Because of this, the effect of the particle collection and extraction process must be considered when evaluating cellular and physiological outcomes upon PM2.5 exposure.

Determination of submicron aerosols effective density using two-stage low-pressure impactor and aerosol electrometer based on pre-measured particle size distribution

A novel methodology was presented for determining the representative effective density of aerosols of a given size distribution, using a lab-made two-stage low-pressure impactor and an aerosol electrometer. Electrical currents upstream (Imeasured, up) and downstream (Imeasured, down) of the 2nd stage of the impactor were measured using a corona charger and the aerosol electrometer. In addition, the electrical currents upstream (Icalculated, up) and downstream (Icalculated, down) of the 2nd stage of the impactor were calculated using the aerosol charging theory. Then, the difference between the ratio of Imeasured,down to Imeasured,up and the ratio of Icalculated,down to Icalculated,up was iterated with varying the presumed effective density until the difference was smaller than 0.001. The methodology was validated using poly-disperse sodium chloride (NaCl) particles. The effective densities of ambient aerosols were then obtained from indoor and outdoor environments and compared with those calculated from a relation between mobility (scanning mobility particle sizer (SMPS) measurement) and aerodynamic (electrical low-pressure impactor (ELPI) measurement) diameters. Compared to the effective densities obtained with SMPS and ELPI measurements, the effective densities obtained using the methodology introduced in this paper differed within 10 % deviation, depending on measurement location. After an averaged effective density for given size distribution is obtained at a measurement location, the number-based size distribution can be easily converted to mass-based size distribution using the representative effective density.

Analysis and classification of individual ambient aerosol particles with field-deployable laser-induced breakdown spectroscopy platform

Analysis and classification of individual ambient aerosol particles with field-deployable laser-induced breakdown spectroscopy platform

Source contribution of black carbon aerosol during 2020–2022 at an urban site in Indo-Gangetic Plain

The extensive emissions of black carbon (BC) from the Indo-Gangetic Plain (IGP) region of India have been well recognized. Particularly, biomass emissions from month-specific crop-residue burning (April, May, October, November) and heating activities (December–February) are considered substantial contributors to BC emissions in the IGP. However, their precise contribution to ambient BC aerosol has not been quantified yet and remains an issue of debate. Therefore, this study aims to fill this gap by quantifying the contribution of these month-specific biomass emissions to ambient BC at an urban site in IGP. This study presents the analysis of BC mass concentrations (MBC) measured for 3 years (2020−2022) in Delhi using an optical photometer i.e., continuous soot monitoring system (COSMOS). A statistical analysis of monthly mean MBC and factors affecting the MBC (ventilation coefficients, air mass back trajectories, fire counts) is performed to derive month-wise contribution due to background concentration, conventional emission, regional transport, crop-residue burning, and heating activities. The yearly mean MBC (5.3 ± 4.7, 5.6 ± 5.0, and 5.3 ± 3.5 μg m−3 during 2020, 2021, and 2022, respectively) remained relatively consistent with repetitive monthly patterns in each year. The peak concentrations were observed from November to January and low concentrations from June to September. Anthropogenic activities contributed significantly to MBC over Delhi with background concentration contributing only 30 % of observed MBC. The percentage contribution of emissions from crop-residue burning varied from 15 % (May) to 37 % (November), while the contribution from heating activities ranged from 25 % (December) to 39 % (January). This source quantification study highlights the significant impact of month-specific biomass emissions in the IGP and can play a vital role in better management and control of these emissions in the region.

Measurement report: A comparison of ground-level ice-nucleating-particle abundance and aerosol properties during autumn at contrasting marine and terrestrial locations

Abstract. Ice-nucleating particles (INPs) are an essential class of aerosols found worldwide that have far-reaching but poorly quantified climate feedback mechanisms through interaction with clouds and impacts on precipitation. These particles can have highly variable physicochemical properties in the atmosphere, and it is crucial to continuously monitor their long-term concentration relative to total ambient aerosol populations at a wide variety of sites to comprehensively understand aerosol–cloud interactions in the atmosphere. Hence, our study applied an in situ forced expansion cooling device to measure ambient INP concentrations and test its automated continuous measurements at atmospheric observatories, where complementary aerosol instruments are heavily equipped. Using collocated aerosol size, number, and composition measurements from these sites, we analyzed the correlation between sources and abundance of INPs in different environments. Toward this aim, we have measured ground-level INP concentrations at two contrasting sites, one in the Southern Great Plains (SGP) region of the United States with a substantial terrestrially influenced aerosol population and one in the Eastern North Atlantic Ocean (ENA) region with a primarily marine-influenced aerosol population. These measurements examined INPs mainly formed through immersion freezing and were performed at a ≤ 12 min resolution and with a wide range of heterogeneous freezing temperatures (Ts above −31 °C) for at least 45 d at each site. The associated INP data analysis was conducted in a consistent manner. We also explored the additional offline characterization of ambient aerosol particle samples from both locations in comparison to in situ data. From our ENA data, on average, INP abundance ranges from ≈ 1 to ≈ 20 L−1 (−30 °C ≤ T ≤ −20 °C) during October–November 2020. Backward air mass trajectories reveal a strong marine influence at ENA with 75.7 % of air masses originating over the Atlantic Ocean and 96.6 % of air masses traveling over open water, but analysis of particle chemistry suggests an additional INP source besides maritime aerosols (e.g., sea spray aerosols) at ENA. In contrast, 90.8 % of air masses at the SGP location originated from the North American continent, and 96.1 % of the time, these air masses traveled over land. As a result, organic-rich SGP aerosols from terrestrial sources exhibited notably high INP abundance from ≈ 1 to ≈ 100 L−1 (−30 °C ≤ T ≤ −15 °C) during October–November 2019. The probability density function of aerosol surface area-scaled immersion freezing efficiency (ice nucleation active surface site density; ns) was assessed for selected freezing temperatures. While the INP concentrations measured at SGP are higher than those of ENA, the ns(T) values of SGP (≈ 105 to ≈ 107 m−2 for −30 °C ≤ T ≤ −15 °C) are reciprocally lower than ENA for approximately 2 orders of magnitude (≈ 107 to ≈ 109 m−2 for −30 °C ≤ T ≤ −15 °C). The observed difference in ns(T) mainly stems from varied available aerosol surface areas, Saer, from two sites (Saer,SGP &gt; Saer,ENA). INP parameterizations were developed as a function of examined freezing temperatures from SGP and ENA for our study periods.

Significant changes in the physicochemical properties of BC-containing particles during the cold season in Beijing

The ambient air quality has improved significantly under strict emission controls in Beijing, China over the last decade. Black carbon (BC), as a short-lived climate forcer in ambient aerosols, profoundly impacts the air quality and climate. Previous studies have demonstrated a decline in the mass concentration of BC. In this study, we characterized the chemical compositions and size distributions of BC-containing particles during the cold season of 2022 in Beijing using state-of-the-art instruments capable of exclusively measuring BC-containing particles. The optical properties of BC-containing particles were further calculated based on the Mie theory. Moreover, we compared the properties of BC-containing particles in 2022 with the results of previous studies. The results showed that the diameters of BC cores became larger while the coating thickness of BC-containing particles became thinner in 2022. For the coating materials, the mass fraction of nitrate increased obviously, and even replaced organic matter as the dominant component during the peak of the pollution period. Variations in chemical compositions and size distributions resulted in lower mass absorption cross-sections (MAC) of BC-containing particles from 10.5 ± 1.1 m2/g in 2016 to 7.3 ± 0.8 m2/g in 2022, reduced by 30.5%. Our results demonstrate the synergistic benefits of air pollution control in improving air quality and mitigating climate change. Therefore, the MAC of BC adopted in climate models should vary with the changing air pollution levels. This study emphasizes that it is imperative to conduct long-term observations of BC-containing particles to better estimate BC's climate effects.

Complex Hygroscopic Behavior of Ambient Aerosol Particles Revealed by a Piezoelectric Technique.

Understanding the complex interactions between atmospheric aerosols and water vapor in subsaturated regions of the atmosphere is crucial for modeling and predicting aerosol-cloud-radiation-climate interactions. However, the microphysical mechanisms of these interactions for ambient aerosols remain poorly understood. For this study, size-resolved samples were collected from a high-altitude, relatively clean site situated in the Western Ghats of India during the monsoon season, in order to study background and preindustrial processes as a baseline for climate functioning within the context of the most polluted region of the world. Measurements of humidity-dependent mass-based growth factors, hygroscopicity, deliquescence behavior, and aerosol liquid water content (ALWC) were made by a novel approach using a quartz crystal microbalance based on a piezo-electric sensor. The climate-relevant fine-mode aerosols (≤2.5 μm) exhibited strong size-dependent variations in their interactions with water vapor and contributed a high fraction of ALWC. Deliquescence occurred for relatively large aerosols (diameter >180 nm) but was absent for smaller aerosols. The deliquescence relative humidity for ambient aerosols was significantly lower than that of pure inorganic salts, suggesting a strong influence of organic species. Our study establishes an improved approach for accurately measuring aerosol water uptake characteristics of ambient aerosols in the subsaturated regime, aiding in the assessment of radiative forcing effects and improving climate models.