Cloud Condensation Nuclei Activity Research Articles

Aerosol Properties and Their Influences on Marine Boundary Layer Cloud Condensation Nuclei over the Southern Ocean

Five overcast marine stratocumulus cases during the Southern Ocean Clouds Radiation Aerosol Transport Experimental Study (SOCRATES) aircraft field campaign were selected to examine aerosol and cloud condensation nuclei (CCN) properties with cloud influence. The Aitken- and accumulation-mode aerosols contributed approximately 70% and 30% of the total aerosols, respectively. The aerosol properties before and after periods of drizzle were investigated using in situ measurements during one case. Sub-cloud drizzle processes impacted accumulation-mode aerosols and CCN distribution. There was a nearly linear increase in CCN number concentration (NCCN) with supersaturation (S) during the ‘before drizzle’ period, but this was not true for the ‘after drizzle’ period, particularly when S > 0.4%. Using the hygroscopicity parameter (κ) to quantitatively investigate the chemical cloud-processing mechanisms, we found that higher κ values (>0.4) represent cloud-processing aerosols, while lower κ values (<0.1) represent newly formed aerosols. When the supersaturation is less than the Hoppel minimum (0.22%), cloud processing is dominant, whereas sea-spray aerosols are dominant contributors to CCN activation when S exceeds 0.22% but is less than 0.32%, the effective supersaturation threshold. Sea salt is considered a non-cloud-processing aerosol and is large and hygroscopic enough to form cloud droplets.

Rapid growth and high cloud-forming potential of anthropogenic sulfate aerosol in a thermal power plant plume during COVID lockdown in India

The COVID lockdown presented an interesting opportunity to study the anthropogenic emissions from different sectors under relatively cleaner conditions in India. The complex interplays of power production, industry, and transport could be dissected due to the significantly reduced influence of the latter two emission sources. Here, based on measurements of cloud condensation nuclei (CCN) activity and chemical composition of atmospheric aerosols during the lockdown, we report an episodic event resulting from distinct meteorological conditions. This event was marked by rapid growth and high hygroscopicity of new aerosol particles formed in the SO2 plume from a large coal-fired power plant in Southern India. These sulfate-rich particles had high CCN activity and number concentration, indicating high cloud-forming potential. Examining the sensitivity of CCN properties under relatively clean conditions provides important new clues to delineate the contributions of different anthropogenic emission sectors and further to understand their perturbations of past and future climate forcing.

Characterization of dust-related new particle formation events based on long-term measurement in the North China Plain

Abstract. Mineral dust is a major natural atmospheric aerosol that impacts the Earth's radiation balance. The significant scavenging process of fine particles by the strong wind during the dust episodes provided a relatively clean environment that was favourable for new particle formation (NPF) occurrence. In this study, the NPF occurred following the dust episodes (dust-related NPF), and other cases under clean and polluted conditions were classified based on the long-term particle number size distribution (PNSD) in urban Beijing in spring from 2017 to 2021. It was found that the observed formation (Jobs) and growth rate (GR) of dust-related NPF events were approximately 50 % and 30 % lower than the values of other NPF days, respectively. A typical severe dust storm that originated from Mongolia and swept over northern China on 15–16 March 2021 was analysed, to illustrate how the dust storm influences the NPF event. The maximum hourly mean PM10 mass concentration reached 8000 µg m−3 during this dust storm. The occurrence of an NPF event after a dust storm was facilitated due to the low condensation sink (∼ 0.005 s−1) caused by the strong dilution process of pre-existing particles. However, a downward trend of particle hygroscopicity was found during dust storm and NPF event as compared with the polluted episode, resulting in an increasing trend of the critical diameter at different supersaturations (ss), where aerosols are activated as cloud condensation nuclei (CCN), although the NPF event occurred when dust faded. The critical diameter was elevated by approximately 6 %–10 % (ss = 0.2 % and 0.7 %) during the dust storm, resulting in a lower CCN activation ratio, especially at low supersaturation. Modifications of the nucleation and growth process, as well as the particle-size distribution and hygroscopicity of the dust particles, provide valuable information that reveals the underlying climate and air quality effects of Asian mineral dust.

Optical properties and cloud condensation nuclei activity of brown carbon containing α–dicarbonyls and reduced nitrogen compounds

The aqueous–phase reaction of carbonyls with reduced nitrogen compounds (RNCs) is considered an important pathway for the formation of secondary BrC, and these particles could greatly impact the global climate. However, our knowledge of their properties is still limited. In this study, we measured the optical properties, cloud condensation nuclei (CCN) activity (represented as hygroscopicity parameter κCCN), and effective density (ρeff) under varied reaction conditions for BrC mixtures formed by reactions between two α–dicarbonyls (glyoxal GX and methylglyoxal MG) and three RNCs (ammonium sulfate AS, glycine GC, and dimethylamine DA). Our results showed a wide range of particle ρeff from 1.08 to 1.66 g cm−3, depending on the type of RNCs reactant. At 532 nm wavelength, the real part n of complex refractive index ranged from 1.41 to 1.60 and the imaginary part k of BrC ranged from 0.024 to 0.043, and the absorption cross section for MG mixtures were 20.3–51.0% higher than those of GX mixtures. These values did not appear to vary significantly with mixing molar ratios between RNCs and α–dicarbonyls (10:1, 1:1, and 1:3) for mixtures with the same reactants, but the mass absorption cross section for mixtures after a reaction time of 14 days were 1.57–74.2% higher than those of mixtures after reaction times of 0.5 and 7 days. The κCCN values of different BrC were consistent with the order of κCCN for single RNCs, i.e., AS–containing (0.349–0.428) > GC–containing (0.221–0.352) > DA–containing (0.090–0.131), and showed an overall increasing trend (1.47–59.3%) with the RNCs content. Our results highlight the importance of reaction conditions on secondary BrC properties and are helpful for a more accurate assessment of aerosol radiative forcing.

Cloud condensation nuclei activation properties of Mediterranean pollen types considering organic chemical composition and surface tension effects

Wind-dispersed pollen grains emitted from vegetation are directly injected into the atmosphere being an important source of natural aerosols globally. These coarse particles of pollen can rupture into smaller particles, known as subpollen particles (SPPs), that may act as cloud condensation nuclei (CCN) and affect the climate. In this study, we characterize and investigate the ability of SPPs of 10 Mediterranean-climate pollen types to activate as CCN. A continuous flow CCN counter (CCNC) was used to measure the activation of size-selected (80, 100 and 200 nm dry mobility diameter) particles at different supersaturations (SS). Hygroscopicity parameter (κ) for each SPP type and size has been calculated using κ-Köhler theory. Organic chemical speciation and protein content has been determined to further characterize pollen solutions. Furthermore, the surface activity of SPPs has also been investigated by using pendant drop tensiometry. All studied SPP samples show critical supersaturation (SSCrit) values that are atmospherically relevant SS conditions. Hygroscopicity κ values are in the range characteristic of organic compounds (0.1–0.3). We found that organic speciation and protein content vary substantially among pollen types, with saccharides and fatty acids being the only organic compounds found in all pollen types. A clear relationship between SPP activation and its organic composition was not observed. This study also reveals that all SPPs investigated reduce the surface tension of water at high concentrations but at diluted concentrations (such as those of activation in the CCNC), the water surface tension value is a good approximation in Köhler theory. Overall, this analysis points out that pollen particles might be an important source of CCN in the atmosphere and should be considered in aerosol-cloud interactions processes.

The impact of particulate pollution control on aerosol hygroscopicity and CCN activity in North China

Air quality has greatly improved in China owing to the strict control policy enforced during the last decade. This study investigated the impact of particulate pollution control on aerosol hygroscopicity and cloud condensation nuclei (CCN) activity in North China based on several data sources. The mass concentration of particles with an aerodynamic diameter smaller than 2.5 µm (PM2.5) decreased by one third from the summer of 2014 to the summer of 2020 in Xinzhou (XZ). The mass fractions of aerosol chemical components in PM2.5 also clearly changed, showing an increase in hydrophilic inorganics and a decrease in hydrophobic organics and black carbon from 2014 to 2020. Measurements of the particle number size distribution in XZ indicate that the occurrence frequency of new particle formation (NPF) events decreased significantly from 2014 to 2020, leading to a reduction in the generation of daytime ultrafine particles. The weakened NPF and increasing influence of morning and evening peak emissions modified the diurnal variations of the number concentration of condensation nuclei (N CN) and CCN (N CCN). The aerosol activation ratio was always higher in the summer of 2014 than in the summer of 2020. These results demonstrate that particulate pollution control can decrease N CN and N CCN but enhance aerosol hygroscopicity and activation ability.

Virus infection of phytoplankton increases average molar mass and reduces hygroscopicity of aerosolized organic matter

Viral infection of phytoplankton is a pervasive mechanism of cell death and bloom termination, which leads to the production of dissolved and colloidal organic matter that can be aerosolized into the atmosphere. Earth-observing satellites can track the growth and death of phytoplankton blooms on weekly time scales but the impact of viral infection on the cloud forming potential of associated aerosols is largely unknown. Here, we determine the influence of viral-derived organic matter, purified viruses, and marine hydrogels on the cloud condensation nuclei activity of their aerosolized solutions, compared to organic exudates from healthy phytoplankton. Dissolved organic material derived from exponentially growing and infected cells of well-characterized eukaryotic phytoplankton host-virus systems, including viruses from diatoms, coccolithophores and chlorophytes, was concentrated, desalted, and nebulized to form aerosol particles composed of primarily of organic matter. Aerosols from infected phytoplankton cultures resulted in an increase in critical activation diameter and average molar mass in three out of five combinations evaluated, along with a decrease in organic kappa (hygroscopicity) compared to healthy cultures and seawater controls. The infected samples also displayed evidence of increased surface tension depression at realistic cloud water vapor supersaturations. Amending the samples with xanthan gum to simulate marine hydrogels increased variability in organic kappa and surface tension in aerosols with high organic to salt ratios. Our findings suggest that the pulses of increased dissolved organic matter associated with viral infection in surface waters may increase the molar mass of dissolved organic compounds relative to surface waters occupied by healthy phytoplankton or low phytoplankton biomass.

Measurement report: High Arctic aerosol hygroscopicity at sub- and supersaturated conditions during spring and summer

Abstract. Aerosol hygroscopic growth and cloud droplet formation influence the radiation transfer budget of the atmosphere and thereby the climate. In the Arctic, these aerosol properties may have a more pronounced effect on the climate compared to the midlatitudes. Hygroscopic growth and cloud condensation nuclei (CCN) concentrations of high Arctic aerosols were measured during two field studies in the spring and summer of 2016. The study site was the Villum Research Station (Villum) at Station Nord in the northeastern region of Greenland. Aerosol hygroscopic growth was measured with a hygroscopic tandem differential mobility analyzer (HTDMA) over a total of 23 d, and CCN concentrations were measured over a period of 95 d. Continuous particle number size distributions were recorded, facilitating calculations of aerosol CCN activation diameters and aerosol κ values. In spring, average CCN concentrations, at supersaturations (SSs) of 0.1 % to 0.3 %, ranged from 53.7 to 85.3 cm−3, with critical activation diameters ranging from 130.2 to 80.2 nm and κCCN ranging from 0.28–0.35. In summer, average CCN concentrations were 20.8 to 47.6 cm−3, while critical activation diameters and κCCN were from 137.1 to 76.7 nm and 0.23–0.35, respectively. Mean particle hygroscopic growth factors ranged from 1.60 to 1.75 at 90 % relative humidity in spring, while values between 1.47 and 1.67 were observed in summer depending on the initial dry size. Although the summer aerosol number size distributions were characterized by frequent new particle formation events, the CCN population at cloud-relevant supersaturations was determined by accumulation-mode aerosols.

Using particle-resolved aerosol model simulations to guide the interpretations of cloud condensation nuclei experimental data

Ambient aerosol particles can undergo dynamic mixing processes as they coagulate with particles from other air masses and emission sources. Therefore, aerosols exist in a spectrum, from externally mixed to internally mixed. The mixing state of aerosols can affect their ability to uptake water (hygroscopicity) and their cloud condensation nuclei (CCN) activity, modifying their contribution to the planet’s total radiative budget. However, current water-uptake measurement methods may not be able to capture the complex mixing state. In this research, the dynamic mixing process was simulated by the particle-resolved aerosol model PartMC and also created by experiments in a laminar flow mixing tube. The mixing evolution of ammonium sulfate and sucrose binary mixtures were observed along with the changes in their water uptake properties expressed as the single hygroscopicity parameter, κ. The use of a mixing simulation in conjunction with experiments allow for better identification of the particle mixing state and the particle water uptake and show that no one kappa value can capture the complexity of mixing across the mixed particle size distribution. In other words, the PartMC simulations can be used as a guiding tool to interpret a system’s mixing state based on its experimental droplet activation spectra. This work demonstrates the importance of the integration and use of mixing models to aid in mixing state determination and hygroscopicity measurements of mixed systems.Copyright © 2023 American Association for Aerosol Research

Solubility Considerations for Cloud Condensation Nuclei (CCN) Activity Analysis of Pure and Mixed Black Carbon Species

Black carbon (BC) is an aerosol that is released into the atmosphere due to the incomplete burning of biomass and can affect the climate directly or indirectly. BC commonly mixes with other primary or secondary aerosols to undergo aging, thereby changing its radiative properties and cloud condensation nuclei (CCN) activity. The composition of aged BC species in the atmosphere is difficult to measure with high confidence, so their associated CCN activity can be uncertain. In this work, the CCN activity analysis of BC was performed using laboratory measurements of proxy aged BC species. Vulcan XC72R carbon black was used as the representative of BC, and three structural isomers of benzenedicarboxylic acid─phthalic acid (PTA), isophthalic acid (IPTA), and terephthalic acid (TPTA)─were mixed with BC to generate three different proxies of aged BC species. Most studies related to CCN activity analysis of BC aerosols use the traditional Köhler theory or an adsorption theory (such as the Frenkel-Halsey-Hill adsorption theory). PTA, IPTA, and TPTA fall in the sparingly water-soluble range and therefore do not fully obey either of the aforementioned theories. Consequently, a novel hybrid activity model (HAM) was used for the CCN activity analysis of the BC mixtures studied in this work. HAM combines the features of adsorption theory via the adsorption isotherm with the features of Köhler theory by incorporating solubility partitioning. The results in this work showed that HAM improves the representation of CCN activity of pure and mixed BC aerosol species with high certainty, evident from generally better goodness of fit, R2 > 0.9. This work implies that the hygroscopicity parameterization based on HAM captures the size-dependent variability in the CCN activity of the pure and aged BC species.

The density of ambient black carbon retrieved by a new method: implications for cloud condensation nuclei prediction

Abstract. The effective density of black carbon (BC) is a crucial factor that is relevant to its aging degree and adds uncertainty in evaluating its climate effect. Here, we have developed a new method to retrieve the effective density of internally mixed BC in the atmosphere, combining field observations conducted from 15 November to 14 December 2016 in urban Beijing with the Köhler theory. The uncertainty in the retrieval method was evaluated to be within ±30 %, which was primarily caused by assumptions on both the hygroscopic parameter of organics and the proportional distribution of primary organic aerosols in different hygroscopic modes. Using the method, we find that the ambient internally mixed BC, accounting for 80 % ± 20 % of total BC aerosol particles, was retrieved with a campaign mean density of 1.1 ± 0.6 g cm−3 during the observed periods. The retrieved result was comparable with that reported in the literature. By applying a lower (0.14 g cm−3) and upper (2.1 g cm−3) limit of the retrieved BC density in the cloud condensation nuclei (CCN) number concentration (NCCN) estimation, we derived that the neglect of such variations in the BC density would lead to an uncertainty of −28 %–11 % in predicting NCCN at supersaturations of 0.23 % and 0.40 %. We also find that the NCCN was more sensitive to the variations in BC density when it was <1.0 g cm−3. This illustrates the necessity of accounting for the effect of BC density on CCN activity closer to source regions where the BC particles are mostly freshly emitted. The CCN closure was achieved when introducing the retrieved real-time BC density and mixing state. This study provides a unique way of utilizing field measurements to infer ambient BC density and highlights the importance of applying variable BC density values in models when predicting CCN and assessing its relevant climate effect.

Aging of α-Pinene Secondary Organic Aerosol by Hydroxyl Radicals in the Aqueous Phase: Kinetics and Products.

The reaction of hydroxyl radicals (OH) with a water-soluble fraction of the α-pinene secondary organic aerosol (SOA) was investigated using liquid chromatography coupled with negative electrospray ionization mass spectrometry. The SOA was generated by the dark ozonolysis of α-pinene, extracted into the water, and subjected to chemical aging by the OH. Bimolecular reaction rate coefficients (kOH) for the oxidation of terpenoic acids by the OH were measured using the relative rate method. The unaged SOA was dominated by the cyclobutyl-ring-retaining compounds, primarily cis-pinonic, cis-pinic, and hydroxy-pinonic acids. Aqueous oxidation by the OH resulted in the removal of early-stage products and dimers, including well-known oligomers with MW = 358 and 368 Da. Furthermore, a 2- to 5-fold increase in the concentration of cyclobutyl-ring-opening products was observed, including terpenylic and diaterpenylic acids and diaterpenylic acid acetate as well as some of the newly identified OH aging markers. At the same time, results obtained from the kinetic box model showed a high degree of SOA fragmentation following the reaction with the OH, which indicates that non-radical reactions occurring during the evaporation of water likely contribute to the high yields of terpenoic aqSOAs reported previously. The estimated atmospheric lifetimes showed that in clouds, terpenoic acids react with the OH exclusively in the aqueous phase. Aqueous OH aging of the α-pinene SOA results in a 10% increase of the average O/C ratio and a 3-fold decrease in the average kOH value, which is likely to affect the cloud condensation nuclei activity of the aqSOA formed after the evaporation of water.

Seasonal variation of particle hygroscopicity and its impact on cloud-condensation nucleus activation in the Beijing urban area

Hygroscopicity is a key parameter for characterizing the ability of particles to be activated as cloud-condensation nuclei (CCN). In this study, we present a 10-month size-resolved measurement of the hygroscopicity of particles with diameters of 50, 100 and 200 nm in the Beijing urban area using a Hygroscopicity-Tandem Differential Mobility Analyzer (H-TDMA). Compared with that in other studies conducted in China, the hygroscopicity parameter (κ) in this study was relatively higher than that in the Pearl River Delta region but lower than that in the Yangtze River Delta region. As the mass fraction of inorganic matter (especially nitrate) increased, the particles became more hygroscopic during spring and summer, as influenced by the chemical composition. Polluted southerly air masses also enhanced particle hygroscopicity. The CCN concentration was calculated based on κ-Köhler theory, with a moderate supersaturation of 0.4%. The critical diameter of particles as potential CCNs was smaller in spring than that in the other seasons. The critical diameters of aerosols in autumn, winter and spring were 142, 123 and 114 nm, respectively, with calculated CCN concentrations of 1683, 1909 and 1765 cm−3, respectively. Activation ratios, calculated as CCN divided by condensation nuclei (CN), were 0.13, 0.15 and 0.18 in autumn, spring and summer, respectively. During episodes of heavy pollution, the CCN concentration highly depended on the particle mass loading, as the accumulation mode dominated the particle number size distribution and the chemical composition was quasi-homogeneous. However, under other conditions, both particle size and chemical composition were important. This study revealed the relationship between particle hygroscopicity, CCN and air pollution level, and it will be useful for evaluating the environmental and climatic effects of aerosols.

Kinetic Limitations Affect Cloud Condensation Nuclei Activity Measurements Under Low Supersaturation

AbstractThe commercial continuous‐flow streamwise thermal‐gradient cloud condensation nuclei (CCN) counter is widely used in aerosol CCN activity measurements which are critical for investigating aerosol‐cloud interactions. In CCN measurements, a critical threshold is needed for distinguishing interstitial aerosols and activated droplets, and a default threshold of 0.75 μm was set in CCN counter. Theoretically, interstitial aerosols could also grow larger than 0.75 μm in CCN counter at low supersaturations, thus theoretical thresholds derived from the Köhler theory were suggested. Here, we report that droplet growth in the CCN counter is kinetically limited and CCN‐active droplets does not reach their theoretical diameters under low supersaturations. Neglecting the kinetic growth limitation in CCN identification would count less CCN and underestimate the aerosol hygroscopicity parameter by up to 50% for supersaturations lower than 0.1%. We recommend that thresholds considering kinetic limitations should be used as new criteria for CCN identification under low supersaturations.

Contrasting Influence of Nitrogen Oxides on the Cloud Condensation Nuclei Activity of Monoterpene‐Derived Secondary Organic Aerosol in Daytime and Nighttime Oxidation

AbstractAnthropogenic nitrogen oxides may influence the cloud condensation nuclei (CCN) activity of biogenic secondary organic aerosols (SOA) in both daytime photooxidation and nighttime NO3 oxidation, which has significant implications for the climatic impact of SOA. We investigated the influence of NOx on the CCN activity of monoterpene‐derived SOA in OH oxidation and in NO3 oxidation. In OH oxidation, NOx had little influence on the hygroscopic parameter κ of organic aerosol (κOrg), which was attributed to the minor fraction of organic nitrates (ON) in SOA (<24%), resulted from the low branching ratio of RO2 + NO to form ON. In contrast, in NO3 oxidation κOrg was much reduced compared to OH/O3 oxidation due to a dominant fraction of ON. We report κ of MT‐derived ON formed in photo‐oxidation and NO3 oxidation (0.029–0.052) for the first time to our knowledge, which may be used to improve model simulations of CCN concentrations.

Influence of aerosol physicochemical properties on CCN activation during the Asian winter monsoon at the summit of Mt. Lu, China

To better understand the characteristics of high-altitude aerosol (or condensation nuclei, CN) and cloud condensation nuclei (CCN) in East China during the Asian winter monsoon, a field campaign focused on aerosol and CCN was set up in the area of Mt. Lu during the period from 5 November to 10 December 2019. The features of CCN and CCN formation at Mt. Lu were analyzed. The CCN spectra at Mt. Lu belongs to a polluted continental type, which could be parameterized using N = 2498S0.31, with S denoting supersaturation. The average and standard deviation of the CCN (S = 0.4%) and CN concentrations were 1936 ± 1007 cm−3 and 3041 ± 1646 cm−3, respectively. The CCN activation fraction (AF) values are 0.43, 0.57, 0.64, 0.69, and 0.72 at S = 0.2%, S = 0.4%, S = 0.6%, S = 0.8% and S = 1%, respectively. The aerosol composition would be more important than aerosol size in determining CCN activation at Mt. Lu. The CCN (CN) number concentration had a clear diurnal variation with maximal and minimal values at 13:00 (12:00 and 18:00) and 07:00 (07:00), respectively. Nearly 68.7% of the air mass reaching Mt. Lu came from the northern area. The higher-sulfate-ratio air mass has a relatively high AF efficiency.

Explicitly Modeling the Effects of Cloud Condensation Nuclei on Warm Rain Initiation

Abstract A bin (or spectral) model is developed to investigate the sensitivity of warm rain initiation to cloud condensation nuclei (CCN). It explicitly represents CCN with a formula whose parameters come from the Twomey relationship (or CCN measurements). By seamlessly integrating CCN activation and drop collection with thousands of bins, the model can replicate the effect of CCN on rain initiation, providing a benchmark to test the process parameterizations in rain initiation. The model is used to simulate two extreme cases with CCN parameters of maritime and continental clouds, respectively, where other actual cases usually lie between these two extreme cases. Its simulations show that rain can initiate within half an hour or less as observed in cumulus clouds. The fast rain initiation modeled is attributed mainly to a new process: the condensational conversion of cloud drops to raindrops via collision–coalescence initiators (or drops with radius between 28 and 100 μm). Since the new process is more important in rain initiation than the autoconversion of cloud drops to raindrops when large CCN exist, it is suggested that the process be parameterized into the weather and climate models to better represent CCN and subsequently remove the common bias of “too dense clouds.” Significance Statement The current weather and climate models represent aerosols via implicit parameterizations and have a bias of “too dense clouds.” Their implicit parameterizations of aerosols usually overlook (or misrepresent) some cloud processes. In this paper and its preceding part (Zeng and Li 2020) we proposed a new framework to explicitly parameterize one subset of aerosols: cloud condensation nuclei (CCN). To embody an explicit parameterization of CCN, we still need quantitative information to connect CCN activation and rain initiation, which motivates this study. In the study we developed an accurate microphysical model to simulate the growth of small CCN to large raindrops, providing information on the sensitivity of rain initiation to CCN. We performed many sensitivity simulations and found the condensational conversion of cloud drops to raindrops via collision–coalescence initiators is a vital process in warm rain initiation. Since the process has been overlooked by all the weather and climate models, the study suggests that the process be introduced in the weather and climate models to properly represent the fast warm rain initiation observed and subsequently remove the bias of “too dense clouds.”

Changes in CCN activity of ship exhaust particles induced by fuel sulfur content reduction and wet scrubbing

Maritime transport remains a large source of airborne pollutants, including exhaust particles that can act as cloud condensation nuclei (CCN).

Reconsideration of surface tension and phase state effects on cloud condensation nuclei activity based on the atomic force microscopy measurement

Abstract. Dicarboxylic acids are ubiquitous in atmospheric aerosol particles, but their roles as surfactants in cloud condensation nuclei (CCN) activity remain unclear. In this study, we investigated CCN activity of inorganic salt (sodium chloride and ammonium sulfate) and dicarboxylic acid (including malonic acid (MA), phenylmalonic acid (PhMA), succinic acid (SA), phenylsuccinic acid (PhSA), adipic acid (AA), pimelic acid (PA), and octanedioic acid (OA)), mixed particles with varied organic volume fractions (OVFs), and then directly determined their surface tension and phase state at high relative humidity (over 99.5 %) via atomic force microscopy (AFM). Our results show that CCN-derived κCCN of studied dicarboxylic acids ranged from 0.003 to 0.240. A linearly positive correlation between κCCN and solubility was obtained for slightly dissolved species, while negative correlation was found between κCCN and molecular volume for highly soluble species. For most inorganic salts and dicarboxylic acids (MA, PhMA, SA, PhSA and PA), a good closure within 30 % relative bias between κCCN and chemistry-derived κChem was obtained. However, κCCN values of inorganic salt–AA and inorganic salt–OA systems were surprisingly 0.3–3.0 times higher than κChem, which was attributed to surface tension reduction, as AFM results showed that their surface tensions were 20 %–42 % lower than that of water (72 mN m−1). Meanwhile, semisolid phase states were obtained for inorganic salt–AA and inorganic salt–OA and also affected hygroscopicity closure results. Our study highlights that surface tension reduction should be considered when investigating aerosol–cloud interactions.

Variations of aerosol and cloud vertical characteristics based on aircraft measurements in upstream of Shanghai during the 2020 China international import expo

Vertical information about aerosols and clouds is vital to understanding aerosol transport, aerosol-cloud interactions, and pollution-weather-climate feedback so as to reduce uncertainties in estimating their climatic effects. The combination of sounding, lidar, aircraft, and satellite measurements is widely used to obtain the vertical information of aerosols and clouds. We used an aircraft measurement over southern Anhui, the upstream regions of Shanghai, on 1 November which conducted to ensure good air quality for the Third China International Import Expo to examine the vertical characteristics of aerosol and cloud microphysical properties and their variations before and after cloud seeding. Observations showed aerosols and clouds were vertically stratified. Most aerosols trapped within the boundary layer are small particles with sizes less than 0.12 µm. Aerosol number concentrations (Na) generally decreased with altitude in the cloudless atmosphere, with the largest particles occurring in 2500–3500 m due to dust transported from distant regions and high ambient humidity. Four separate cloud layers with unequal depths dominated by altostratus and nimbostratus appeared at different heights. The maximum cloud droplet concentration (Nc) and the minimum cloud droplet diameter (Dc) that appeared in the mid-level cloud (2246–2482 m) were 107.7 cm−3 and 4.03 μm, respectively, owing to the high proportion of hygroscopic particles. Hygroscopic particles played an important role in the growth of droplets and the activation of cloud condensation nuclei, especially under high ambient humidity. Cloud droplet size spectrum showed a unimodal distribution with a single peak at 5 µm in low- (970–1000 m) and mid-level clouds, but a trimodal distribution with peaks at 7 μm, 12 μm, and 17 μm in the mid-high- and high-level clouds, indicating the broadening of spectra with increasing altitude. An artificial seeding experiment was conducted in the high-level clouds. Big cloud droplets and ice crystals increased significantly after cloud seeding. Meanwhile, cloud particle populations showed less Nc, larger Dc, and a wider size spectrum. Our results suggest that the artificial precipitation experiment promoted rainfall to a certain extent and contributed to the removal of pollutants from upstream regions, which is beneficial to the air quality of Shanghai.