Aerosol Hygroscopicity Research Articles

Effect of Long‐Range Transported Fire Aerosols on Cloud Condensation Nuclei Concentrations and Cloud Properties at High Latitudes

AbstractActive vegetation fires in south‐eastern (SE) Europe resulted in a notable increase in the number concentration of aerosols and cloud condensation nuclei (CCN) particles at two high latitude locations—the SMEAR IV station in Kuopio, Finland, and the Zeppelin Observatory in Svalbard, high Arctic. During the fire episode aerosol hygroscopicity κ slightly increased at SMEAR IV and at the Zeppelin Observatory κ decreased. Despite increased κ in high CCN conditions at SMEAR IV, the aerosol activation diameter increased due to the decreased supersaturation with an increase in aerosol loading. In addition, at SMEAR IV during the fire episode, in situ measured cloud droplet number concentration (CDNC) increased by a factor of ∼7 as compared to non‐fire periods which was in good agreement with the satellite observations (MODIS, Terra). Results from this study show the importance of SE European fires for cloud properties and radiative forcing in high latitudes.

Measurement report: Hygroscopicity of size-selected aerosol particles in the heavily polluted urban atmosphere of Delhi: impacts of chloride aerosol

Abstract. Recent research has revealed the crucial role of wintertime, episodic high chloride (H-Cl) emissions in the Delhi region, which significantly impact aerosol hygroscopicity and aerosol-bound liquid water, thus contributing to the initiation of Delhi fog episodes. However, these findings have primarily relied on modeled aerosol hygroscopicity, necessitating validation through direct hygroscopicity measurements. This study presents the measurements of non-refractory bulk aerosol composition of PM1 from an Aerodyne aerosol chemical speciation monitor and for first-time size-resolved hygroscopic growth factors (nucleation, Aitken, and accumulated mode particles) along with their associated hygroscopicity parameters at 90 % relative humidity using a hygroscopic tandem differential mobility analyzer at the Delhi Aerosol Supersite. Our observations demonstrate that the hygroscopicity parameter for aerosol particles varies from 0.00 to 0.11 (with an average of 0.03 ± 0.02) for 20 nm particles, 0.05 to 0.22 (0.11 ± 0.03) for 50 nm particles, 0.05 to 0.30 (0.14 ± 0.04) for 100 nm particles, 0.05 to 0.41 (0.18 ± 0.06) for 150 nm particles, and 0.05 to 0.56 (0.22 ± 0.07) for 200 nm particles. Surprisingly, our findings demonstrate that the period with H-Cl emissions displays notably greater hygroscopicity (0.35 ± 0.06) in comparison to spans marked by high biomass burning (0.18 ± 0.04) and high hydrocarbon-like organic aerosol (0.17 ± 0.05) and relatively cleaner periods (0.27 ± 0.07). This research presents initial observational proof that ammonium chloride is the main factor behind aerosol hygroscopic growth and aerosol-bound liquid water content in Delhi. The finding emphasizes ammonium chloride's role in aerosol–water interaction and related haze/fog development. Moreover, the high chloride levels in aerosols seem to prevent the adverse impact of high organic aerosol concentrations on cloud condensation nuclei activity.

Measurement report: Water diffusion in single suspended phase-separated aerosols

Abstract. Water diffusion is a typical thermodynamic process in ambient aerosols that plays pivotal roles in their physicochemical properties and atmospheric lifetime and influences the climate and human health. A fair amount of aerosols become phase-separated after experiencing atmospheric aging processes such as efflorescence, amorphization, and liquid–liquid phase separation. However, detecting the hygroscopicity of heterogeneous aerosols is quite intractable. Here, for the first time, we directly characterized the water diffusion in single suspended phase-separated aerosols via a self-constructed laser tweezer Raman spectroscopy (LTRS) system. The H2O–D2O isotope exchange was harnessed to trace the water diffusion in single laser-levitated homogenous/heterogeneous microdroplets. The time-resolved cavity-enhanced Raman spectra of the microdroplets were used to detect the diffusion process in real time. Two archetypes of phase-separated aerosols, i.e., partially engulfed and core–shell, were studied. Moreover, we quantified the dynamic water diffusion process by experimentally measuring the diffusion coefficients. The results showed that compared with the homogenous aerosols, water diffusion limitations existed in the phase-separated aerosols. The incomplete diffusion may stem from the formation of certain hydrated molecule clusters. This work provides possible implications for the evolutions, especially the gas–particle partition, of the actual phase-separated atmospheric aerosols.

Causes of an extremely low visibility event in Northeast China

AbstractAn extreme haze‐fog event occurred during October 20–22, 2013, in Harbin, Northeast China, which lasted for nearly 60 h with local visibility as low as 20 m. However, causes of the extreme haze‐fog formation remain unclear. Through the analysis of in situ data and objective weather circulation classification, it is revealed that high pollutant emissions from biomass burning played a very important role in the extreme event. Stable weather conditions under the circulation type 8 (CT8), marked by weak high‐pressure control, strong inversion (6.55°C), shallow boundary layer depth (<300 m), and high relative humidity (>90%), aided in the accumulation of pollutants and hygroscopic aerosol growth. All of these factors collectively contributed to the extreme haze‐fog formation. The insights derived from this study can improve the predictability of extreme haze‐fog events, and indicate that pollution emissions should be tightly controlled in the adverse meteorological circulation type in Northeast China.

Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning

Abstract. In this study we investigated the photo-oxidation of Euro 5 gasoline vehicle emissions during cold urban, hot urban and motorway Artemis cycles. The experiments were conducted in an environmental chamber with average OH concentrations ranging between 6.6 × 105–2.3 × 106 molec. cm−3, relative humidity (RH) between 40 %–55 % and temperatures between 22–26 °C. A proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) and the CHemical Analysis of aeRosol ON-line (CHARON) inlet coupled with a PTR-ToF-MS were used for the gas- and particle-phase measurements respectively. This is the first time that the CHARON inlet has been used for the identification of the secondary organic aerosol (SOA) produced from vehicle emissions. The secondary organic gas-phase products ranged between C1 and C9 with one to four atoms of oxygen and were mainly composed of small oxygenated C1–C3 species. The SOA formed contained compounds from C1 to C14, having one to six atoms of oxygen, and the products' distribution was centered at C5. Organonitrites and organonitrates contributed 6 %–7 % of the SOA concentration. Relatively high concentrations of ammonium nitrate (35–160 µg m−3) were formed. The nitrate fraction related to organic nitrate compounds was 0.12–0.20, while ammonium linked to organic ammonium compounds was estimated only during one experiment, reaching a fraction of 0.19. The SOA produced exhibited log C∗ values between 2 and 5. Comparing our results to theoretical estimations for saturation concentrations, we observed differences of 1–3 orders of magnitude, indicating that additional parameters such as RH, particulate water content, aerosol hygroscopicity, and possible reactions in the particulate phase may affect the gas-to-particle partitioning.

Impact of SO2 and light on chemical morphology and hygroscopicity of natural salt aerosols

The interactions between SO2 and natural salt aerosol particles represent complex and crucial dynamics within atmospheric processes and the broader climate system. This study investigated the SO2 uptake, hygroscopicity, morphology and mixing states of natural salt particles, which are generated from brines sampled from the Chaka salt lake located in the Qinghai-Tibet plateau. A comparison with atomized pure NaCl particles is included as reference. The results show that NaCl particles exhibit the lowest SO2 uptake, while Chaka salt particles demonstrate higher uptake due to their complex composition. The hygroscopicity of salt particles is influenced by several factors, including chemical complexity, SO2 exposure and light conditions. In comparison to pure NaCl, Chaka salt displays higher hygroscopicity, which is further enhanced in the presence of SO2. However, when exposed to light, mass growth is suppressed, suggesting the formation of species with lower hygroscopicity, such as Na2SO4. Analysis of particle morphology and mixing states reveals notable distinctions between NaCl crystals and Chaka salt particles, where the Chaka salt particles exhibit rounded shapes with a structure composed of cubic NaCl cores surrounded by sulfate materials as a coating. In addition, the chemical morphology analysis also reveals that the particles show morphological and spectral changes before and after the exposure to SO2, light and high RH. Therefore, this research highlights the intricate interactions between SO2 and natural salt aerosol particles in diverse environmental settings, underscoring their multifaceted impacts on atmospheric processes.

The influence of aerosol hygroscopicity on clouds and precipitation over Western Ghats, India

AbstractWe examine the role of aerosol hygroscopicity (κ) on the formation of clouds and precipitation over the Western Ghats (WG) in India using various numerical model simulations (i.e., particle‐by‐particle‐based small‐scale, high‐resolution mesoscale model). For the diffusional growth of cloud droplets, the size‐dependent hygroscopicity is used in the κ‐Köhler equation of direct numerical simulation. The results of the small‐scale model reveal that the distribution of cloud drop size varies from the initial mixing state to the well‐mixed state due to variation in κ. The value of κ is obtained from Humidified Tandem Differential Mobility Analyzer (HTDMA) instruments at the High Altitude Cloud Physics Laboratory, India. The idealized and real simulations using the Weather and Research Forecasting (WRF) model with the aerosol‐aware Thompson microphysics scheme are conducted by changing κ values. Depending on the type of clouds (shallow or deep), different κ values determine the mass and number of cloud and rain droplets. Low hygroscopicity (organics) simulates more and smaller drops, as well as uplifts below freezing level, resulting in more ice‐phase hydrometeors. Organic aerosols have a significant impact on the formation of more snow and graupel hydrometeors. As compared to high κ, low hygroscopicity weakens updrafts at the intermediate level and strengthens them at the upper level in the deep cloud region. The intensity of precipitation varies due to low and high κ. The findings indicate that aerosol composition has a significant impact on the activation of cloud condensation nuclei. This study suggests that aerosol hygroscopicity is essential in weather prediction models to integrate aerosol chemical compositions.

Impacts of variations in aerosol refractive index on the retrieving of the light-absorption and hygroscopicity of ambient black carbon-containing aerosols using SP2

Black carbon (BC) aerosols directly influence the earth's climate system by absorbing the light intensity and indirectly by interacting with clouds. The microphysical properties of BC-containing aerosols were determined by their core diameter and shell thickness, which can be derived from the measurement of a single-particle soot photometer (SP2). Traditionally, a constant real part of the shell's refractive index (RRI) was employed to retrieve the shell thickness of BC-containing aerosols using the measured scattering signals from SP2. Recent field measurements in East China show that ambient aerosol RRI varies over a wide range between 1.36 and 1.56. The influences of aerosol RRI variation on the retrieving of BC-containing aerosol shell thickness from the measurements of SP2 are investigated with simulation studies. Results show that the variation in ambient aerosol RRI can lead to a variation in the coating thickness of BC-containing aerosols by 9.4%. The corresponding uncertainties in the light absorption enhancement reach up to 29% due to the influence of aerosol RRI. The critical mean supersaturation (SS) of the BC-containing aerosol varies significantly between 0.044% and 0.055% due to the uncertainties in the derived shell thickness using a constant RRI. This study highlights the demand for the real-time measurement of ambient aerosol RRI when deriving the microphysical properties of ambient BC-containing aerosols from the SP2 measurement.

Highly Hygroscopic Aerosols Facilitate Summer and Early‐Autumn Cloud Formation at Extremely Low Concentrations Over the Central Arctic Ocean

AbstractArctic clouds are sensitive to atmospheric particles since these are sometimes in such low concentrations that clouds cannot always form under supersaturated water vapor conditions. This is especially true in the late summer, when aerosol concentrations are generally very low in the high Arctic. The environment changes rapidly around freeze‐up as the open waters close and snow starts accumulating on ice. We investigated droplet formation during eight significant fog events in the central Arctic Ocean, north of 80°, from August 12 to 19 September 2018 during the Arctic Ocean 2018 expedition onboard the icebreaker Oden. Calculated hygroscopicity parameters (κ) for the entire study were very high (up to κ = 0.85 ± 0.13), notably after freeze‐up, suggesting that atmospheric particles were very cloud condensation nuclei (CCN)‐active. At least one of the events showed that surface clouds were able to form and persist for at least a couple hours at aerosol concentrations less than 10 cm−3, which was previously suggested to be the minimum for cloud formation. Among these events that were considered limited in CCN, effective radii were generally larger than in the high CCN cases. In some of the fog events, droplet residuals particles did not reactivate under supersaturations up to 0.95%, suggesting either in‐droplet reactions decreased hygroscopicity, or an ambient supersaturation above 1%. These results provide insight into droplet formation during the clean late‐summer and fall of the high Arctic with limited influence from continental sources.

CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California

Abstract. The UNIfied Partitioning-Aerosol phase Reaction (UNIPAR) model was integrated into the Comprehensive Air quality Model with extensions (CAMx) to process secondary organic aerosol (SOA) formation by capturing multiphase reactions of hydrocarbons (HCs) in regional scales. SOA growth was simulated using a wide range of anthropogenic HCs, including 10 aromatics and linear alkanes with different carbon lengths. The atmospheric processes of biogenic HCs (isoprene, terpenes, and sesquiterpene) were simulated for major oxidation paths (ozone, OH radicals, and nitrate radicals) to predict day and night SOA formation. The UNIPAR model streamlined the multiphase partitioning of the lumping species originating from semi-explicitly predicted gas products and their heterogeneous chemistry to form non-volatile oligomeric species in both organic aerosol and inorganic aqueous phase. The CAMx–UNIPAR model predicted SOA formation at four ground urban sites (San Jose, Sacramento, Fresno, and Bakersfield) in California, United States, during wintertime 2018. Overall, the simulated mass concentrations of the total organic matter, consisting of primary organic aerosol and SOA, showed a good agreement with the observations. The simulated SOA mass in the urban areas of California was predominated by alkane and terpene oxidation products. During the daytime, low-volatility products originating from the autoxidation of long-chain alkanes considerably contributed to the SOA mass. In contrast, a significant amount of nighttime SOA was produced by the reaction of terpene with ozone or nitrate radicals. The spatial distributions of anthropogenic SOA associated with aromatic and alkane HCs were noticeably affected by the southward wind direction, owing to the relatively long lifetime of their atmospheric oxidation, whereas those of biogenic SOA were nearly insensitive to wind direction. During wintertime 2018, the impact of inorganic aerosol hygroscopicity on the total SOA budget was not evident because of the small contribution of aromatic and isoprene products, which are hydrophilic and reactive in the inorganic aqueous phase. However, an increased isoprene SOA mass was predicted during the wet periods, although its contribution to the total SOA was little.

Current challenges in the visibility improvement of urban Chongqing in Southwest China: From the perspective of PM2.5-bound water uptake property over 2015–2021

The visibility (VIS) improvement remains challenging such as in Southwest China, although the aerosol loading was reduced markedly. More in-depth understanding of interactions between visibility and aerosol physicochemical properties is required. This study systematically investigated mechanisms behind the interannual variation of low visibility at urban Chongqing from the aspect of PM2.5-bound optical enhancements over a relatively large timescale of 2015–2021. Results show that VIS <10 km frequently exceeded 50% in 2021 despite remarkable emission reductions since 2015, with the most severe challenge in visibility improvement faced in winter. Generally, the annual mean aerosol hygroscopicity and light extinction capacity were promoted during 2015–2021, as demonstrated by a higher optical enhancement factor (f(RH)), aerosol liquid water content per unit PM2.5 mass (i.e., ALWC/PM2.5), and dry mass extinction efficiency (MEEdry) observed for 2021 in comparison to previous years. A pronounced ascending trend existed in the annual mean fraction of nitrate (fNO3−), which even surpassed organics and sulfate to be the predominant composition in PM2.5. A similar evolution of fNO3− was observed during the visibility degradation specifically when VIS <10 km, highlighting the importance of highly hydrophilic inorganics in the haze formation. Given that the higher level of fNO3− normally introduced an elevated ALWC/PM2.5 which likely enhanced secondary aerosol formation (e.g., sulfate, nitrate, and secondary organics) via multiphase reactions, the combined effects could further exacerbate the visibility degradation particularly under highly humid and polluted conditions. Stricter controls such as on NOx and volatile organic precursors would be beneficial for the visibility improvement in China.

The technical innovation of integrating the gold mesh sampling method into FTIR spectroscopy, along with its application in the domain of transportation-related pollution studies, signifies a noteworthy advancement in analytical capabilities

Recently, Fourier transform infrared micro-spectroscopy (FTIR) has played a crucial role in the study of heterogeneous reactions in atmospheric chemistry. This includes research on aerosol hygroscopicity, nucleation kinetics, chemical composition analysis of aerosols, and heterogeneous chemical reactions on aerosol particle surfaces. This paper presents a novel approach that introduces a gold mesh during the sampling process, enabling the true spectrum of liquid water to be measured in transmission mode, thereby addressing spectral distortion issues at 3400 cm-1. Additionally, common inorganic components of atmospheric pollution were measured, providing a feasible method for using FTIR spectroscopy to address atmospheric pollution issues. Finally, the introduction of the gold mesh sampling method was employed to measure the heterogeneous chemical kinetics of road dust surface during traffic pollution processes, offering a viable solution for using FTIR spectroscopy to address atmospheric pollution concerns.

Application of physisorption analyzer in measuring the hygroscopicity of atmospheric aerosols

The hygroscopicity represents a vital physicochemical attribute of aerosols, governing their phase state, acidity, viscosity, chemical reactivity, and other properties, thereby influencing various atmospheric processes, including visibility, radiative forcing, and the formation of cloud condensation nuclei. In this study, the hygroscopicity of common inorganic aerosol particles (NH4)2SO4 and NaCl in the atmosphere was determined using a physisorption analyzer under 298 K conditions, exploring its application prospects in measuring atmospheric aerosol hygroscopicity. By measuring the adsorption of particles to water vapor at different relative humidity (RH) levels, the variation curve of the aerosol particle hygroscopic mass growth factor (MGF) and deliquescence relative humidity (DRH) were obtained. Comparisons with vacuum FTIR methods, the Extended Aerosol Inorganic Model (EAIM), and relevant literature data showed good agreement. This research paves the way for future applications of physisorption analyzer in the study of atmospheric aerosols.

Changes in wintertime visibility across China over 2013–2019 and the drivers: A comprehensive assessment using machine learning method

Effective emission reduction measures have largely lowered the particulate concentration in China, but low-visibility events still occur frequently, greatly affecting people's daily life, travel, and health. In the context of carbon neutrality strategy and climate change, the mechanisms governing visibility changes may be undergoing a transformation. To address this critical issue, we have undertaken a comprehensive assessment by employing a novel approach that combines site observations, model-derived datasets, and machine learning techniques. Our analysis of the dataset shows varying degrees of improvement in wintertime visibility in regions such as North China, South China, and the Fenwei Plain over 2013–2019, but an unexpected deterioration (approximately 1 km yr−1) in central and southern China (CSC). We further elucidate key roles of PM2.5 reduction in these regions with visibility improvement; whereas the unsatisfactory visibility trend in CSC was caused by combined effect of relative humidity (RH) increase (47 %), aerosol hygroscopicity (κ) enhancement (9 %), and boundary layer (BLH) reduction (8 %), which greatly overwhelms the effect of PM2.5 reduction recently. Moreover, the study reveals a growing influence of RH on the wintertime visibility, reaching 40 % ± 24 % to the total contribution in 2019, while that of PM2.5 declined to 18 % ± 19 % and is expected to further diminish with emission reduction. Note those often-neglected factors-temperature, wind speed, BLH, and κ, account for over 40 % of the total contribution. Though the importance of aerosol hygroscopic growth to visibility was found decreasing recently, it retains non-negligible impacts on driving inter-annual visibility trends. This study yields innovative insights for air pollution control, underscoring the imperative of region-specific strategies to mitigate low-visibility events.

On the Chemical Composition and Hygroscopicity of Aerosols Deposited on the Insulators of Italian Power Lines

The reliability of the national power grid is a key issue in modern society. Atmospheric aerosols are the main cause of the reduction in the performance of insulators and the increase in the possibility of flashovers, resulting in power line failures. Under high ambient humidity, the water-soluble compounds of atmospheric aerosols collected on the insulators’ surface can dissociate in ions and form a conductive layer, which may lead to flashover events. With a view to investigating the processes that drive these phenomena, the chemical composition of aerosol deposits on insulators in Italy was determined by ion chromatography analysis and thermos-optical and X-ray techniques. In addition, a synthetic aerosol with the same analyzed chemical composition was generated in a laboratory and deposited on PTFE filters and glass specimens allowing us to determine the deliquescence and crystallization relative humidity and the conductive effect in an aerosol exposure chamber. The results evidenced the presence of a hazardous inorganic ion layer, which generates a sharp phase transition of the aerosol deposit as a function of the ambient relative humidity; this layer poses a dangerous threat to the reliability of the power grid, increasing the probability of flashover events where the conductive layer facilitates the flow of electrical current across the insulator surface, potentially causing power outages or damage to the power lines.

The effects of aerosol concentration on the evolution, transport, and deposition of hygroscopic droplets in the highly idealized MT model: A numerical study

Inhalation therapy is widely used to treat various respiratory diseases. Nebulizers have been widely adopted due to their ease of operation, high drug delivery efficiency, and low residual volume. Traditional studies on drug delivery in the respiratory tract typically use a one-way coupled method to track drug transport and deposition for non-hygroscopic drug particles. However, neglecting the concentration of nebulized hygroscopic droplet aerosols can lead to significant discrepancies in the deposition efficiency (DE) of nebulized drugs in the airways. To investigate the effect of different nebulization rates on the evolution, transport, and deposition of droplets, a highly idealized mouth-throat (MT) model was selected as a testbed for the in silico trials of drug delivery to the respiratory tract. The interaction between continuous and discrete phases was modeled using a two-way coupled model of highly concentrated droplet aerosol-water vapor interaction, innovated by the particle parcel method. The effects of different coupling methods and boundary conditions on the average droplet diameter and droplet deposition distribution pattern at the outlet of the MT model were compared using a computational fluid dynamics (CFD) method. Simulation results indicate that neglecting the effect of water vapor evaporated from the droplets on the relative humidity (RH) in the oral cavity could lead to a 2.2-fold prediction error of the average droplet diameter at the outlet of the MT model for a conventional nebulization rate of 0.386 g/min. As the nebulization rate increases, the difference in the predicted average droplet diameter at the outlet of the MT model between the one-way coupled method and the two-way coupled method also increases. Increasing the nebulization rate during inhalation therapy could lead to incomplete evaporation of drug droplets, resulting in deposition of larger diameter drug droplets in the oral cavity. In contrast, a lower nebulization rate can reduce the droplet diameter at the outlet of the MT model, allowing it to enter deeper airways.

Single‐Scattering Properties of Encapsulated Fractal Black Carbon Particles Computed Using the Invariant Imbedding T‐Matrix Method and Deep Learning Approaches

AbstractEfficient and accurate computation of the single‐scattering properties of black carbon (BC) aerosols is fundamental in various fields, including remote sensing and climate simulations. In this study, we developed a composite model of fractal aggregates of BC encapsulated with hygroscopic aerosols to represent the ambient BC. We used the invariant imbedding T‐matrix method to compute the optical properties of fully and partially encapsulated BC aerosols. In this new model, the traditional assumption of unoverlapped surfaces in the super‐position T‐matrix method is unnecessary. After extensive simulations, we established a database of single‐scattering properties, including the extinction efficiency, the single‐scattering albedo, the asymmetry factor and six phase matrix elements. Moreover, we obtained deep neural networks (DNNs) from this database using a deep learning method. These DNN models provide a universal interface for predicting the optical properties of ambient BC aerosols. Specifically, through a modified architecture of the DNN, we trained two models based on the database to predict three integrated optical properties (extinction efficiency, single‐scattering albedo, and asymmetry factor) and six phase matrix elements. We performed statistical assessments based on the true values in the database and the predicted values from the DNNs, demonstrating that the DNNs accurately predicted all single‐scattering properties. Therefore, the developed DNN models can be conveniently implemented in aerosol optical parameterization for remote sensing studies and atmospheric models.

Significant impact of water-soluble organic matter on hygroscopicity of fine particles under low relative humidity condition

Uncertainties in estimating the hygroscopicity of bulk aerosols under conditions of low relative humidity (RH) or below the deliquescent RH (DRH) of aerosols remain to be significant, mainly due to the presence of water-soluble organic matter (WSOM). To quantify the contributions of WSOM to aerosol hygroscopicity and associated uncertainties, a field campaign was conducted to measure the hygroscopic growth curve (f(RH)) of bulk aerosols online, dominant chemical compositions in PM2.5 online and offline, and size distributions of the dominant chemical compositions offline during the dry and wet seasons of 2019–2020 in urban Guangzhou of south China. Based on the measured f(RH), the hygroscopicity parameter (κ) of bulk aerosols (κ-f(RH)) exhibits a logarithmic increase with increasing RH until RH reaches 69 %. Beyond this threshold, κ-f(RH) increases very slowly with further increase of RH, reaching 0.32 ± 0.04 during the dry season and 0.31 ± 0.05 during the wet season. The κ of WSOM (κ-WSOM) was further estimated to be 0.22 ± 0.03 and 0.13 ± 0.04 in the dry and wet seasons, respectively, when RH > 69 %. WSOM significantly affects κ-f(RH) by retarding the deliquescence process of aerosols and altering the mass ratio of water-soluble inorganic salts (WSIS) to WSOM within the size range of 0.4–0.9 μm, especially under low RH conditions (<60 %). The κ-f(RH) under low RH conditions was revised based on the logarithmic regression equation between RH and the ratio of measured κ-f(RH) to estimated κ-f(RH>69%). f(RH) of WSIS and WSOM were then corrected using the revised κ-f(RH) under low RH conditions, which showed 22–31 % lower values than those produced by the IMPROVE formulas.

Global organic and inorganic aerosol hygroscopicity and its effect on radiative forcing

The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵorg) and inorganic ions (ϵinorg) through a linear combination, κ = ϵorg ⋅ κorg + ϵinorg ⋅ κinorg. In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κorg = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κorg and κinorg is small, we constrain a critically important aspect of global climate modelling.

Characteristics of atmospheric boundary layer and its relation with PM2.5 during winter in Shihezi, an Oasis city in Northwest China

Based on low-level atmospheric meteorological elemental and pollutant data in the vertical direction observed during a tethered sonde sounding experiment from December 27, 2019 to January 14, 2020 this study analysed the atmospheric boundary layer vertical structure and its influence on winter PM2.5 concentrations in Shihezi City, Xinjiang, using Richardson number (Ri) profiling and correlation analysis to better understand the correlation between the atmospheric boundary layer structure and continuous heavy pollution in Shihezi City during winter. The results showed that heavy pollution continued during the observational period, and the diurnal variation in the atmospheric boundary layer disappeared. The atmospheric boundary layer structure tended to remain stable, and the average boundary layer height was only 109 m. The lengthy temperature inversion lifespan, high humidity, and low-wind layer near the surface primarily contributed to the sustained heavy pollution during winter in Shihezi City. Temperature and wind speed during heavy pollution events were negatively correlated with the PM2.5 concentrations in the near-surface layer. Stable atmospheric thermodynamic stratification with a cold lower layer and a warm upper layer in the atmospheric boundary layer weakens vertical atmospheric pollutant diffusion. Moreover, increased relative humidity (RH) is beneficial for hygroscopic aerosol particle growth and liquid-phase chemical reactions, thus worsening heavy pollution.