Hygroscopicity Parameter Research Articles

Interaction of cesium compounds with abundant inorganic compounds of atmosphere: Effect on cloud formation potential and settling.

Experiments were conducted in controlled laboratory conditions to determine the size-resolved CCN (Cloud Condensation Nuclei) activity of sub micrometer-sized aerosols containing nuclear fission products (CsI and CsOH) and abundant ambient inorganic aerosols ammonium sulphates ((NH4)2SO4), ammonium chloride (NH4Cl), sodium nitrate (NaNO3), and sodium chloride (NaCl). The presence of these atmospheric-relevant compounds internally mixed with fission product compounds has the potential to affect the capacity of ambient particulates of aerosols to absorb water and function as CCN. Once in the atmosphere, the dynamics of airborne radionuclides and subsequently their fate gets affected by dry and wet deposition processes. The interplay of source and decay terms determines the transit of radioactivity and impacts its local and/or global spread. After being exposed to a sufficiently humid atmosphere, released cesium particles have a high potential to act as CCN. However, the CCN properties of the resulting mixed particles may be altered due to their interaction with atmospheric particles. DMT-CCN counter was used to acquire CCN activation curves with initial dry particle size variation (20-300 nm) for mixed particles (ratio 1:1) at 0.1-1 % supersaturation (SS). For a variety of particle sizes and mixtures of soluble materials, activation ratio curves were obtained under various SS conditions. From the study of CCN spectra, an estimate of the hygroscopicity parameter (κ) was made, which is sensitive to the chemical composition of aerosols. Under different SS conditions, the CCN activation diameters of mixed aerosols were found to be affected greatly in comparison to pure compounds. For the first time, the spectral efficiency of CCNs and the activation diameters of CsI and CsOH particles combined with important atmospheric aerosols were described at various SS levels. Terminal settling velocities for the mixed particles having a representative diameter as critical activation droplet diameter (wet diameter at particular SS), and varying effective density (based on droplet composition) were obtained and compared with the pure state of particles at different SS levels. The relative difference was significant for some combinations and SS conditions. Any modification in settling velocity ultimately impacts the particle's lifetime and deposition flux estimations. Hence neglecting the presence of atmospheric salts affects the accuracy of the source term estimates for a postulated nuclear reactor accident scenario. Data on these features is crucial for modelling the behavior of these particles in simulations. In the extremely improbable event of a containment breach occurring under severe nuclear accident conditions, the outcome has the potential to enhance environmental source-term estimations.

Cloud drop activation of insoluble aerosols aided by film-forming surfactants

Abstract. Cloud droplet activation of insoluble aerosols covered by insoluble surfactant films has been studied theoretically by combining the FHH (Frenkel–Halsey–Hill) activation theory and an equation of state suitable for surfactant films that are in an expanded state. The key parameters governing the ability of the surfactant to suppress critical supersaturations are its partial molecular area at the water surface and the size of the molecule. For a fixed size, molecules with a larger molecular area are more efficient, whereas with a fixed area-to-volume ratio smaller molecules are more efficient. Calculations made for stearic acid films on black carbon and illite aerosols indicate that the critical supersaturations are significantly lower than with pure particles, especially when the dry particle sizes are several hundred nanometers and larger. Furthermore, the reductions in critical supersaturation are similar when stearic acid is replaced by water-soluble organics with values of the hygroscopicity parameter (κ) of up to 0.5. However, mixtures of surfactant and water-soluble organic compounds are relatively weaker at reducing critical supersaturations than either of these compounds alone, which is caused by dilution of the surfactant film as the dissolved organic causes increased uptake of water vapor in the critical droplets. The theory has also been tested against experimental results on the impact of oleic acid films on the activation of calcite particles.

Multiwavelength Raman lidar system for profiling the CCN number concentrations

Cloud condensation nuclei (CCN) play an important role in the research of cloud microphysical and aerosol–cloud interactions. This study employs a multiwavelength Raman lidar for measuring CCN concentration. First, the multiwavelength Raman lidar was used to measure the atmospheric relative humidity profile, and the combination of relative humidity and the aerosol backscattering coefficient was used to retrieve the hygroscopic growth factor. By fitting the hygroscopic growth factor using the κkappa parameter model, the hygroscopic parameter κkappa that characterizes the hygroscopicity of aerosols was obtained. Then, the critical activation radius of aerosols was derived using the κ–Köhler theory and hygroscopicity parameter κkappa. Finally, the CCN number concentration was obtained by combining with the aerosol particle size distribution. Experiments were conducted to verify the feasibility of the multiwavelength Raman lidar. Results showed that the effective detection range of the lidar is approximately 0–4 km. The error of the temperature measured by the lidar at the height of 0.3–3.8 km is approximately ±1K. When the relative humidity change is 0.77–0.87, the range of the hygroscopic growth factor change is 1.06–1.10, the hygroscopic parameter γ is 0.065, and the hygroscopic parameter κkappa is 0.009. The CCN numbers concentration decreases with height but increases closer to the cloud. The multiwavelength Raman lidar is an important tool for detection of cloud microphysical and aerosol–cloud interactions and could have scientific importance and research value, both for improved understanding of the formation of clouds and precipitation and for enhanced accuracy of weather modification.

Deriving the hygroscopicity of ambient particles using low-cost optical particle counters

Abstract. This study investigates the chemical composition and physical properties of aerosols, which play a crucial role in influencing human health, cloud physics, and local climate. Our focus centers on the hygroscopicity of ambient aerosols, a key property reflecting the ability to take up moisture from the atmosphere and serve as cloud condensation nuclei. Employing home-built air quality box (AQB) systems equipped with low-cost sensors, we assess the ambient variability of particulate matter (PM) concentrations to determine PM hygroscopicity. The AQB systems effectively captured meteorological parameters and most pollutant concentrations, showing high correlations with data from the Taiwan Environmental Protection Administration (TW-EPA). With the application of κ-Köhler equation and certain assumptions, AQB-monitored PM concentrations are converted to dry particle mass concentration, providing optical particle counter sensitivity correction and resulting in improved correlation with TW-EPA data. The derived single hygroscopicity parameters (κ) range from 0.15 to 0.29 for integrated fine particles (PM2.5) and 0.05 to 0.13 for coarse particles (PM2.5−10), consistent with results of ionic chromatography analysis from a previous winter campaign nearby. Moreover, the analysis of PM10 division into PM2.5 and PM2.5−10, considering composition heterogeneity, provided improved dry PM10 concentration as the sensitivity coefficients for PM2.5−10 were notably higher than for PM2.5. Our methodology provides a comprehensive approach to assess ambient aerosol hygroscopicity, with significant implications for atmospheric modeling, particularly in evaluating aerosol efficiency as cloud condensation nuclei and in radiative transfer calculations. Overall, the AQB systems proved to be effective in monitoring air quality and deriving key aerosol properties, contributing valuable insights into atmospheric science.

Multiple-charging effects on the CCN activity and hygroscopicity of surrogate black carbon particles

Accurate measurements of cloud condensation nuclei (CCN) activity and hygroscopicity of black carbon (BC)-containing particles are particularly important because of the positive climate forcing from these particles. Such measurements are typically conducted on particles selected by a Differential Mobility Analyzer (DMA), which in addition to singly charged particles transmits multiply charged larger particles that have the same electrical mobility. These larger particles activate at lower supersaturations than the singly charged particles, biasing measurements and resulting in overestimation of CCN activity and hygroscopicity parameter (κ). Here, we measure the CCN activity and determine κ for different BC surrogates with electrical mobility diameters from 100 to 200 nm selected 1) only by electrical mobility with a DMA, and 2) by both electrical mobility and mass using a DMA and a Centrifugal Particle Mass Analyzer (CPMA), thus allowing selection of only singly charged particles. We demonstrate the use of the DMA-CPMA system in resolving biases caused by multiply charged particles, and we show that the effect of multiple charging on the CCN activity of the BC particles is strongly influenced by morphology dispersion, i.e., the variability due to the range of morphologies of particles that have the same electrical mobility and mass. Our findings show that electrical mobility-based methods alone are unlikely to lead to accurate results in measurements of CCN activation and hygroscopicity of BC particles, even for those with a more compact morphology.

Aerosol mixing state, new particle formation, and cloud droplet number concentration in an urban environment

Anthropogenically derived aerosols have been hypothesized to influence convective precipitation by increasing the available pool of cloud condensation nuclei. Here, we present a synthesis of aerosol size distribution and subsaturated hygroscopicity measurements between 15 and 250 nm diameter particles during the TRacking Aerosol Convection interactions ExpeRiment (TRACER). We found that the aerosol is externally mixed and can be described by a quasi-two-component description comprising a more and less hygroscopic mode. The mean hygroscopicity parameters for these modes across all sizes were 0.03 ± 0.04 and 0.22 ± 0.08 with no significant dependence on particle size. The number fraction of the more hygroscopic mode is 40 % for particles between 15 and 40 nm and gradually increases to ~70 % for particles >100 nm. Winds from the southerly direction feature particles with larger hygroscopicity parameters and have a larger fraction of particles in the more hygroscopic mode. The hygroscopicity parameter exhibits diurnal cycles that are consistent with condensation of a species with a hygroscopicity parameter ~0.1 which corresponds to values expected for secondary organic aerosol. We also identified nine small particle events that were attributed to particle formation by nucleation. The data are consistent with new particle formation having occurred aloft, followed by downward mixing with daytime turbulence. The species that are responsible for modal growth had hygroscopicity parameters varying between 0.05 and 0.34. These values systematically depended on the wind sector, suggesting that the chemical composition of the precursors differed. Hourly cloud condensation nuclei (CCN) and cloud droplet number concentration (CDNC) values derived from the aerosol size distribution, subsaturated hygroscopicity measurements, and adiabatic parcel model simulations showed a dynamic range of a factor of 2–3 in CDNC depending on the wind sector, with lower values associated with southerly onshore flow.

Chebyshev–Ritz and Navier's methods for hygro‐magneto vibration of Euler–Bernoulli nanobeam resting on Winkler–Pasternak elastic foundation

AbstractThis research employs Chebyshev–Ritz method along with Navier's method to investigate the vibration characteristics of a nanobeam subject to a longitudinal magnetic field and linear hygroscopic environment. The nanobeam is characterized by a Winkler–Pasternak elastic foundation and follows the nonlocal Euler–Bernoulli beam theory. The governing equation of motion is derived using Hamilton's principle, and non‐dimensional frequency parameters are computed for Simply Supported‐Simply Supported (SS), Clamped‐Clamped (CC), and Clamped‐Free (CF) boundary conditions. The motivation behind this study is to provide a comprehensive and efficient analytical framework for understanding the dynamic behavior of nanobeams in complex environments. By investigating the influence of magnetic and hygroscopic factors on the vibration characteristics of nanobeams, this research aims to offer valuable insights for the design and optimization of nanoscale structures. Employing shifted Chebyshev polynomials as shape functions in Chebyshev–Ritz method offers several advantages in the proposed model. Firstly, these polynomials possess orthogonal properties, which can significantly enhance computational efficiency. The orthogonality of shifted Chebyshev polynomials allow for simpler and more streamlined numerical computations compared to non‐orthogonal basis functions. Additionally, the orthogonality ensures that the resulting system of equations is well‐conditioned, even for higher‐order polynomial approximations. A closed‐form solution for SS boundary condition is obtained through Navier's method. Convergence analysis is performed to validate the accuracy and effectiveness of the proposed model against existing models. The non‐dimensional frequency parameters obtained using both Navier's method and Chebyshev–Ritz method demonstrate strong agreement, further validating the proposed nanobeam model. Additionally, a comprehensive parametric study evaluates the impact of various characteristics, including the small‐scale parameter, Winkler modulus, shear modulus, magnetic parameter, and hygroscopic parameter. The findings contribute to a nuanced understanding of nanobeam vibrations under the influence of a magnetic field and hygroscopic environment, providing valuable insights for the design and optimization of nanoscale structures in practical applications.

Low Hygroscopicity of Newly Formed Particles on the North China Plain and Its Implications for Nanoparticle Growth

AbstractThe growth of newly formed particles through new particle formation (NPF) contributes a significant fraction to the cloud condensation nuclei, yet the driving mechanisms remain unclear, especially for polluted environments. To investigate the potential species contributing for nanoparticle growth in environments with significant anthropogenic influences, we measured the hygroscopicity of newly formed particles at 20–40 nm at a rural observational site in the North China Plain during winter 2018. Our results demonstrate that these particles were not very hygroscopic, with the mean hygroscopicity parameter κ of 0.13 ± 0.09. Clear differences in the inferred κ of the growing material responsible for the growth were observed among different events, indicating that even at the same region, the compounds driving particle growth may not be identical. This may be synergistically influenced by the NPF precursors, oxidants and meteorological conditions, suggesting complex mechanisms might co‐exist behind nanoparticle growth in polluted environments.

Dissecting PM sensor capabilities: A combined experimental and theoretical study on particle sizing and physicochemical properties

Recent advancements in particulate matter (PM) optical measurement technology have enhanced the characterization of particle size distributions (PSDs) across various temporal and spatial scales, offering a more detailed analysis than traditional PM mass concentration monitoring. This study employs field experiments, laboratory tests, and model simulations to evaluate the influence of physicochemical characteristics of particulate matter (PM) on the performance of a compact, multi-channel PM sizing sensor. The sensor is integrated within a mini air station (MAS) designed to detect particles across 52 channels. The field experiments highlighted the sensor's ability to track hygroscopicity parameter κ-values across particle sizes, noting an increasing trend with particle size. The sensor's capability in identifying the size and mass concentration of different PM types, including ammonium nitrate, sodium chloride, smoke, incense, and silica dust particles, was assessed through laboratory tests. Laboratory comparisons with the Aerodynamic Particle Sizer (APS) showed high consistency (R2 > 0.96) for various PM sources, supported by Kolmogorov-Smirnov tests confirming the sensor's capability to match APSsize distributions. Model simulations further elucidated the influence of particle refractive index and size distributions on sensor performance, leading to optimized calibrant selection and application-specific recommendations. These comprehensive evaluations underscore the critical interplay between the chemical composition and physical properties of PM, significantly advancing the application and reliability of optical PM sensors in environmental monitoring.

Additive Water Uptake of the Mixtures of Urban Atmospheric HULIS and Ammonium Sulfate

AbstractThe hygroscopicity of atmospheric aerosols affect the global climate and human health. However, the hygroscopic behavior of mixtures of inorganic salts and organics in atmospheric aerosols have not been well characterized for ambient complex organic mixtures. Here, the hygroscopic growth of humic‐like substances (HULIS), which represent the complexity of organic aerosol compounds, from urban aerosols and their mixtures with ammonium sulfate were investigated with measurements from a hygroscopicity tandem differential mobility analyzer and model analyses. The Zdanovskii–Stokes–Robinson (ZSR) relationship, which assumes that the water uptake of each component is additive, was examined for the mixtures. The dependence of the hygroscopicity parameters (κ) of the mixtures on the volume fraction of HULIS is generally represented by the ZSR relationship with the deviations of κ on average of 16% (4%–27% in different mixing ratios), and 0.03 (0.02–0.04) on absolute basis. An assumption of asphericity for the dry particles reduced the deviations (14%). Approximations for the surface tension depression by surfactants and surface‐bulk partitioning were predicted to account for the deviations to a small extent. Furthermore, a thermodynamic model for simplified compound systems showed that the non‐ideality of the solutions potentially explained the deviations from the ZSR relationship. The results of this study support the use of the ZSR relationship for organic‒inorganic mixtures as a practical approximation in atmospheric models, provide a guide for the uncertainty associated with this approximation, and suggest directions for future studies.

Impact of Anthropogenic Aerosol Transport on Cloud Condensation Nuclei Activity During Summertime in Qilian Mountain, in the Northern Tibetan Plateau

AbstractIn this study, we conducted field campaigns at two mountain‐top observatories on the Qilian Mountains (QLM) in the northeastern Tibetan Plateau of China, which plays a vital role in sustaining water resources for the downstream arid and semi‐arid regions. The two observatories, Waliguan Baseline Observatory (WLG) and Laohugou station (LHG), are situated on the eastern and western edge of the QLM, respectively. The objectives of this study were to examine the properties of atmospheric aerosols, CCN concentrations (NCCN) at varying supersaturation levels (SS = 0.2%–1.0%), and the hygroscopic nature of aerosols in the QLM, especially during the formation of orographic cloud. Notably, the average aerosol concentration and NCCN was approximately 2–3 factors higher at WLG compared to LHG. The chemical compositions of aerosols were primarily dominated by sulfate and organic aerosol (OA) at these two sites. A very high hygroscopicity parameter of aerosol calculated using chemical composition was observed at these two sites (0.37 ± 0.03 at LHG vs. 0.30 ± 0.04 at WLG). Enhanced aerosol loading episodes impacted by anthropogenic emission were observed at these two sites. Exploration on high‐loading cases at each site, we found that the CCN activity was dominated by aerosol size, but the chemical processes of aerosol during the formation of orographic cloud could also be important in CCN activity, especially for low SS conditions. These findings collectively underscore the significant impact of anthropogenic air plumes on CCN concentrations in the QLM and their potential influence on precipitation patterns.

Impact of Biomass Burning on Arctic Aerosol Composition.

Emissions from biomass burning (BB) occurring at midlatitudes can reach the Arctic, where they influence the remote aerosol population. By using measurements of levoglucosan and black carbon, we identify seven BB events reaching Svalbard in 2020. We find that most of the BB events are significantly different to the rest of the year (nonevents) for most of the chemical and physical properties. Aerosol mass and number concentrations are enhanced by up to 1 order of magnitude during the BB events. During BB events, the submicrometer aerosol bulk composition changes from an organic- and sulfate-dominated regime to a clearly organic-dominated regime. This results in a significantly lower hygroscopicity parameter κ for BB aerosol (0.4 ± 0.2) compared to nonevents (0.5 ± 0.2), calculated from the nonrefractory aerosol composition. The organic fraction in the BB aerosol showed no significant difference for the O:C ratios (0.9 ± 0.3) compared to the year (0.9 ± 0.6). Accumulation mode particles were present during all BB events, while in the summer an additional Aitken mode was observed, indicating a mixture of the advected air mass with locally produced particles. BB tracers (vanillic, homovanillic, and hydroxybenzoic acid, nitrophenol, methylnitrophenol, and nitrocatechol) were significantly higher when air mass back trajectories passed over active fire regions in Eastern Europe, indicating agricultural and wildfires as sources. Our results suggest that the impact of BB on the Arctic aerosol depends on the season in which they occur, and agricultural and wildfires from Eastern Europe have the potential to disturb the background conditions the most.

Characterization of size-resolved aerosol hygroscopicity and liquid water content in Nanjing of the Yangtze River Delta

Aerosol hygroscopicity and liquid water content (ALWC) have important influences on the environmental and climate effect of aerosols. In this study, we measured the hygroscopic growth factors (GF) of particles with dry diameters of 40, 80, 150, and 200 nm during the wintertime in Nanjing. Both the GF-derived hygroscopicity parameter (κgf) and ALWC increased with particle size, but displayed differing diurnal variations, with κgf peaking around the midday, while ALWC peaking in the early morning. Nitrate, ammonium and oxygenated organic aerosols (OOA) were found as the chemical components mostly strongly correlated with ALWC. A closure study suggests that during midday photo-oxidation and nighttime high ALWC periods, the κ of organic aerosols (κorg) was underestimated when using previous parameterizations. Accordingly, we re-constructed parameterizations for κorg and the oxidation level of organics for these periods, which indicates a higher hygroscopicity of photochemically formed OOA than the aqueous OOA, yet both being much higher than the generally assumed OOA hygroscopicity. Additionally, in a typical high ALWC episode, concurrently increased ALWC, nitrate, OOA as well as aerosol surface area and mass concentrations were observed under elevated ambient RH. This strongly indicates a coupled effect that the hygroscopic secondary aerosols, in particular nitrate with strong hygroscopicity, led to large increase in ALWC, which in turn synergistically boosted nitrate and OOA formation by heterogeneous/aqueous reactions. Such interaction may represent an important mechanism contributing to enhanced formation of secondary aerosols and rapid growth of fine particulate matter under relatively high RH conditions.

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.

Effects of volatile organic compounds and new particle formation on real-time hygroscopicity of PM2.5 particles in Seosan, Republic of Korea

The hygroscopicity of PM2.5 particles plays an important role in PM2.5 haze in Northeast Asian countries by influencing particle growth and chemical composition. New particle formation (NPF) and atmospheric volatile organic compounds (VOCs) are factors that influence particle hygroscopicity. However, the lack of real-time hygroscopicity measurements has deterred the understanding of their effects on particle hygroscopicity. In this study, two intensive monitoring campaigns were conducted during the summer of 2021 and spring of 2022 using real-time aerosol instruments, including a humidified tandem differential mobility analyzer (HTDMA), in Seosan, Republic of Korea. The hygroscopicity parameter κ was calculated from the real-time HTDMA measurement data (κGf). The diurnal variations in κGf exhibited strong inverse linear correlations with the total concentration of VOCs (CTVOC) during the two campaigns. The higher atmospheric CTVOC in summer increased the growth rate of the particle diameter from 10 to 40 nm (6 nm/h) compared with that in spring (2.7 nm/h), resulting in a faster change in κGf for 40-nm particles in summer than in spring because of the increase in organic matter in the chemical compositions of particles. In addition, NPF events introduced additional tiny fresh particles into the atmosphere, which reduced the κGf of 40-nm particles and increased the intensity of the less hygroscopic peaks (κGf < 0.1) of κ-probability density functions (κ-PDF) in NPF days. However, 100-nm particles exhibited fewer changes in κGf than 40-nm particles, resulting in additional dominant hygroscopic peaks (κ ∼ 0.2) of κ-PDFs in both NPF and non-NPF days. When κGf values measured in Seosan were compared with those in other Northeast Asian countries in the literature, the κ values for 40-nm particles were lower than those (κ > 0.2) measured in Beijing and Guangzhou, but those for 100-nm particles were close to those measured in the two cities.

Particle phase state and aerosol liquid water greatly impact secondary aerosol formation: insights into phase transition and its role in haze events

Abstract. The particle phase state is crucial for reactive gas uptake, heterogeneous, and multiphase chemical reactions, thereby impacting secondary aerosol formation. This study provides valuable insights into the significance of particle-phase transition and aerosol liquid water (ALW) in particle mass growth during winter. Our findings reveal that particles predominantly exist in a semi-solid or solid state during clean winter days with ambient relative humidity (RH) below 30 %. However, a non-liquid to liquid phase transition occurs when the ALW mass fraction exceeds 15 % (dry mass) at transition RH thresholds of 40 %–60 %. During haze episodes, the transformation rates of sulfate and nitrate aerosols rapidly increase through phase transition and increased ALW by 48 % and 11 %, respectively, resulting in noticeable increases in secondary inorganic aerosols (SIA). The presence of abundant ALW, favored by elevated RH and higher proportion of SIA, facilitates the partitioning of water-soluble compounds from the gas to the particle phase, as well as heterogeneous and aqueous processes in liquid particles. This leads to a substantial increase in the formation of secondary organic aerosols and elevated aerosol oxidation. Consequently, the overall hygroscopicity parameters exhibit a substantial enhancement, with a mean value of 23 %. These results highlight phase transition as a key factor initiating the positive feedback loops between ALW and secondary aerosol formation during haze episodes over the North China Plain. Accurate predictions of secondary aerosol formation necessitate explicit consideration of the particle phase state in chemical transport models.

Contrail formation on ambient aerosol particles for aircraft with hydrogen combustion: a box model trajectory study

Abstract. Future air traffic using (green) hydrogen (H2) promises zero carbon emissions, but the effects of contrails from this new technology have hardly been investigated. We study contrail formation behind aircraft with H2 combustion by means of the particle-based Lagrangian Cloud Module (LCM) box model. Assuming the absence of soot and ultrafine volatile particle formation, contrail ice crystals form solely on atmospheric background particles mixed into the plume. While a recent study extended the original LCM with regard to the contrail formation on soot particles, we further advance the LCM to cover the contrail formation on ambient particles. For each simulation, we perform an ensemble of box model runs using the dilution along 1000 different plume trajectories. The formation threshold temperature of H2 contrails is around 10 K higher than for conventional contrails (which form behind aircraft with kerosene combustion). Then, contrail formation becomes primarily limited by the homogeneous freezing temperature of the water droplets such that contrails can form at temperatures down to around 234 K. The number of ice crystals formed varies strongly with ambient temperature even far away from the contrail formation threshold. The contrail ice crystal number clearly increases with ambient aerosol number concentration and decreases significantly for ambient particles with mean dry radii ⪅ 10 nm due to the Kelvin effect. Besides simulations with one aerosol particle ensemble, we analyze contrail formation scenarios with two co-existing aerosol particle ensembles with different mean dry sizes or hygroscopicity parameters. We compare them to scenarios with a single ensemble that is the average of the two aerosol ensembles. We find that the total ice crystal number can differ significantly between the two cases, in particular if nucleation-mode particles are involved. Due to the absence of soot particle emissions, the ice crystal number in H2 contrails is typically reduced by more than 80 %–90 % compared to conventional contrails. The contrail optical thickness is significantly reduced, and H2 contrails either become visible later than kerosene contrails or are not visible at all for low ambient particle number concentrations. On the other hand, H2 contrails can form at lower flight altitudes where conventional contrails would not form.

Roles of marine biota in the formation of atmospheric bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the North Pacific Ocean, Bering Sea, and Arctic Ocean

Abstract. We investigated the association of marine biological indicators (polysaccharides, protein-like gel particles, and chl a) with the formation of fluorescent aerosol particles, cloud condensation nuclei (CCNs), and ice-nucleating particles (INPs) over the North Pacific Ocean, Bering Sea, and Arctic Ocean during September–November 2019. The abundance of bioindicators was high in the North Pacific Ocean and the Bering Sea (e.g., up to 1.3 mg m−3 of chl a), suggesting high biological activity due to a phytoplankton bloom. In the North Pacific Ocean, particles were characterized by high mass fractions of organics and sulfate with a predominance of terrestrial air masses. Conversely, in the Bering Sea and the Arctic Ocean, particles were characterized by high mass fractions of sea salt and sulfate with a predominance of maritime air masses. The averaged range/value of the CCN concentration at 0.4 % supersaturation were 99–151, 43–139, and 36 cm−3 over the North Pacific Ocean with terrestrial influences, over the Bering Sea with marine biogenic influences, and over the Arctic Ocean with marine influences, respectively, and the corresponding range/value of the hygroscopicity parameter κ were 0.17–0.59, 0.42–0.68, and 0.66, respectively. The averaged INP concentration (NINP) measured at temperatures of −18 and −24 ∘C with marine sources in the North Pacific and Bering Sea was 0.01–0.09 and 0.1–2.5 L−1, respectively, and that over the Arctic Ocean was 0.001–0.016 and 0.012–0.27 L−1, respectively. When marine sources were dominant, fluorescent bioaerosols in the fine mode were strongly correlated with all bioindicator types (R: 0.81–0.88) when the effect of wind-induced uplift from the sea surface to the atmosphere was considered. Correlations between NINP measured at −18 and −24 ∘C and all bioindicator types (R: 0.58–0.95 and 0.79–0.93, respectively) were positive, even when the extreme outlier point was omitted, as were those between NINP and fluorescent bioaerosols (R: 0.50 and 0.60, respectively), suggesting that marine bioindicators contributed substantially as sources of bioaerosols and to cloud formation.

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.

Determination of Hygroscopic Aerosol Growth Based on the OPC-N3 Counter

We present the first estimations of single hygroscopic parameter κ for Polish urban area. The results were obtained using an inexpensive OPC-N3 optical particulate matter counter and the ASC 1000 Acoem Aerosol Conditioning System. Our studies were carried out during the winter and spring seasons, between 2020 and 2022 in Warsaw, Poland. We study the difference of κ between these two seasons, as the aerosol has different origins. The mean value of the hygroscopicity parameter for spring (April–June) was 0.13±0.13 and for winter (December-March) it was 0.04±0.04 (obtained using PM1). The mean value of the growth factor for spring (April–June) was 1.52±0.23 and for winter (December–March) it was 1.16±0.13 (obtained using PM1). The values for winter period suggest that during the cold season the aerosol mixture in the atmosphere is dominated by non-hygroscopic particles. However events of higher κ &gt; 0.5 where occurring (mostly for big aerosol particles 1–10 μm in size), when the air mass was coming from North Atlantic carrying sea salt particles. Furthermore, based on κ we propose a method to remove the dependence of PM values on relative humidity on the OPC-N3 optical particulate counter.