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Background and purpose Virus-containing aerosol droplets emitted by breathing, speech or coughing dry rapidly to equilibrium with ambient relative humidity (RH), increasing in solute concentration with effects on virus survival and decreasing in diameter with effects on sedimentation and respiratory uptake. The aim of this paper is to model the effect of ionic and macromolecular solutes on droplet drying and solute concentration. Methods Deliquescence-efflorescence concepts and Kohler theory were used to simulate the evolution of solute concentrations and water activity in respiratory droplets, starting from efflorescence data on mixed NaCl/KCl aerosols and osmotic pressure data on respiratory macromolecules. Results In NaCl/KCl solutions total salt concentrations were shown to reach 10-13 M at the efflorescence RH of 40-55%, depending on the K:Na ratio. Dependence on K:Na ratio implies that the evaporation curves differ between aerosols derived from saliva and from airway surfaces. The direct effect of liquid droplet size through the Kelvin term was shown to be smaller and restricted to the evolution of breath emissions. Modelling the effect of proteins and glycoproteins showed that salts determine drying equilibria down to the efflorescence RH, and macromolecules at lower RH. Conclusion Differences in solute composition between airway surfaces and saliva are predicted to lead to different drying behaviour of droplets emitted by breathing, speech and coughing. These differences may influence the inactivation of viruses.

Size-resolved turbulent fluxes of fog droplets are investigated above a subtropical montane cloud forest in Taiwan. By integrating an aerosol spectrometer into an eddy-covariance set-up, we measure droplet number fluxes and liquid water fluxes in a size range of aerosol particles and droplets with diameters ranging from 0.25 $${\upmu }\!\mathrm{m}$$ μ m to 17.3 $${\upmu }\!\mathrm{m}$$ μ m . We find two flux-direction changes within this size range: a downward flux occurs for accumulation-mode aerosols of diameters between 0.25 $${\upmu }\!\mathrm{m}$$ μ m and 0.83 $${\upmu }\!\mathrm{m}$$ μ m , an upward flux occurs for hydrated aerosols with diameters between 1.1 $${\upmu }\!\mathrm{m}$$ μ m and 2.4 $${\upmu }\!\mathrm{m}$$ μ m , and a downward flux occurs again for activated fog droplets between diameters of 3 $${\upmu }\!\mathrm{m}$$ μ m and 17.3 $${\upmu }\!\mathrm{m}$$ μ m . The droplet size distributions can be modelled by a trimodal log-normal distribution, and the modes correlate with the different flux directions. The formation of the three modes and the establishment of the respective flux directions can be explained by combining the Köhler theory on the basis of measured ion concentrations in fog with the turbulent transport of droplets. Finally, from the combined analysis of droplet fluxes and size distributions, we infer relevant processes of droplet development and dissolving during various phases of the life cycles of the fog events.

A large-eddy simulation model is coupled with a Lagrangian cloud model to study marine fog. In this model, aerosols and droplets are treated from a Lagrangian frame of reference, in contrast to the traditional bulk and bin microphysical models. Droplet growth via condensation is governed by Kohler theory and environmental conditions local to the droplet. Coupling to the vapour and temperature fields of the flow ensures mass, momentum, and energy conservation between the air and droplet phases. Based on the recent C-FOG field campaign, a simulation is performed which highlights the benefits and potential of this type of model. By initializing the simulation with the measured aerosol size distribution and making assumptions about the chemical composition of the multiple peaks, the simulations provide a clear explanation for the observed bimodal droplet distribution during C-FOG: high supersaturation levels cause condensational growth of nearly all coarse-mode aerosols (presumed to be composed of marine salt), as well as a large number of accumulation model aerosols (presumed to be of continental origin with a lower hygroscopicity). The largest peak in the resulting droplet distribution is created from coarse-mode aerosols with high hygroscopicity, while the secondary peak is only possible due to the limited impact of the largest peak on saturation levels inside the fog. Thus, for the simulated levels of supersaturation, it is the limited number of coarse-mode aerosols which is responsible for the emergence of a larger second peak.

Combustion and other high-temperature processes frequently result in the emission of aerosols in the form of polydisperse fractal-like aggregates made of condensed-phase nanoparticles (soot for instance). If certain conditions are met, the emitted aerosol particles are known to evolve into important cloud condensation nuclei (CCN) in the atmosphere. In this work, the hygroscopic parameter κ of complex morphology aggregates is calculated from the supersaturation-dependent activated fraction Fa=Fa(SS) in the frame of κ-Köhler theory. The particle size distribution is approximated with the morphology-corrected volume equivalent diameter calculated from the electrical mobility diameter by taking into account the diameter of the primary particle and the fractal dimension of the aggregate experimentally obtained from transmission electron microscopy measurements. Activation experiments are performed in water supersaturation conditions using a commercial CCN-100 condensation nuclei counter. The model is tested in close-to-ideal conditions of size-selected, isolated spherical particles (ammonium sulfate nanoparticles dispersed in nitrogen), then with complex polydisperse fractal-like aggregates (soot particles activated by exposure to ozone with κ as low as 5×10-5) that represent realistic anthropogenic emissions in the atmosphere.

The Aerodynamic Aerosol Classifier (AAC) is a novel instrument that size-selects aerosol particles based on their mechanical mobility. So far, the application of an AAC for Cloud Condensation Nuclei (CCN) activity analysis of aerosols has yet to be explored. Traditionally, a Differential Mobility Analyzer (DMA) is used for aerosol classification in a CCN experimental setup. A DMA classifies particles based on their electrical mobility. Substituting the DMA with an AAC can eliminate multiple charging artifacts as classification using an AAC does not require particle charging. In this work, we describe an AAC-based CCN experimental setup and CCN analysis method. We also discuss and develop equations to quantify the uncertainties associated with aerosol particle sizing. To do so, we extend the AAC transfer function analysis and calculate the measurement uncertainties of the aerodynamic diameter from the resolution of the AAC. The analyses framework has been packaged into a Python-based CCN Analysis Tool (PyCAT 1.0) open-source code, which is available on GitHub for public use. Results show that the AAC size-selects robustly (AAC resolution is 10.1, diffusion losses are minimal and particle transmission is high) at larger aerodynamic diameters (≥∼85 nm). The size-resolved activation ratio is ideally sigmoidal since no charge corrections are required. Moreover, the uncertainties in the critical particle aerodynamic diameter at a given supersaturation canpropagate through droplet activation and the subsequent uncertainties with respect to the single-hygroscopicity parameter (κ) are reported. For a known aerosol such as sucrose, theκderived from the critical dry aerodynamic diameter can be up to ∼50 % different from the theoretical κ. In this work, we do additional measurements to obtain dynamic shape factor information and convert the sucrose aerodynamic to volume equivalent diameter. The volume equivalent diameter applied to κ- Köhler theory improves the agreement between measured and theoretical κ. Given the limitations of the coupled AAC-CCN experimental setup, this setup is best used for low hygroscopicity aerosol (κ ≤ 0.2) CCN measurements.

The Chilean Coastal Orographic Precipitation Experiment (CCOPE) was a 3-month field campaign (June, July and August 2015) that investigated wintertime coastal rain events. Reported here are analyses of aerosol measurements made at a coastal site during CCOPE. The aerosol monitoring site was located near Arauco, Chile. Aerosol number concentrations and aerosol size distributions were acquired with a condensation particle counter (CPC) and an ultra high sensitivity aerosol spectrometer (UHSAS). Arauco CPC data were compared to values measured at the NOAA observatory Trinidad Head (THD) on the northern Pacific coast of California. The winter-averaged CPC concentration at Arauco is 2971 ± 1802 cm−3; at THD the average is 1059 ± 855 cm−3. Despite the typically more pristine South Pacific region, the Arauco average is larger than at THD (p). Aerosol size distributions acquired during episodes of onshore flow were analyzed with Köhler theory and used to parameterize cloud condensation nuclei activation spectra. In addition, sea salt aerosol (SSA) concentration was parameterized as a function of sea surface wind speed. It is anticipated these parameterizations will be applied in modeling of wintertime Chilean coastal precipitation.

Determination of cloud condensation nuclei (CCN) number concentrations at cloud base is important to constrain aerosol–cloud interactions. A new method to retrieve CCN number concentrations using backscatter and extinction profiles from multiwavelength Raman lidars is proposed. The method implements hygroscopic enhancements of backscatter and extinction with relative humidity to derive dry backscatter and extinction and humidogram parameters. Humidogram parameters, Ångström exponents, and lidar extinction-to-backscatter ratios are then linked to the ratio of CCN number concentration to dry backscatter and extinction coefficient (ARξ). This linkage is established based on the datasets simulated by Mie theory and κ-Köhler theory with in-situ-measured particle size distributions and chemical compositions. CCN number concentration can thus be calculated with ARξ and dry backscatter and extinction. An independent theoretical simulated dataset is used to validate this new method and results show that the retrieved CCN number concentrations at supersaturations of 0.07 %, 0.10 %, and 0.20 % are in good agreement with theoretical calculated values. Sensitivity tests indicate that retrieval error in CCN arises mostly from uncertainties in extinction coefficients and RH profiles. The proposed method improves CCN retrieval from lidar measurements and has great potential in deriving scarce long-term CCN data at cloud base, which benefits aerosol–cloud interaction studies.

Comprehensive field campaigns dedicated to fog life cycle observation were conducted during the winters of 2010–2013 at the Instrumented Site for Atmospheric Remote Sensing Research (SIRTA) observatory in a suburb of Paris. In order to document their properties, in situ microphysical measurements collected during 23 fog events induced by both radiative cooling and stratus lowering are examined here. They reveal large variability in number, concentration and size of both aerosol background before the fog onset and fog droplets according to the different cases. The objective of this paper is to evaluate the impact of aerosol particles on the fog microphysics. To derive an accurate estimation of the actual activated fog droplet number concentration Nact, we determine the hygroscopicity parameter κ, the dry and the wet critical diameter and the critical supersaturation for each case by using an iterative procedure based on the κ-Köhler theory that combines cloud condensation nuclei (CCN), dry particle and droplet size distribution measurements. Our study reveals low values of the derived critical supersaturation occurring in fog with a median of 0.043 %. Consequently, the median dry and wet activation diameters are 0.39 and 3.79 µm, respectively, leading to a minor fraction of the aerosol population activated into droplets. The corresponding Nact values are low, with median concentrations of 53.5 and 111 cm−3 within the 75th percentile. The activated fraction of aerosols exhibits remarkably low correlation with κ values, which reflects the chemical composition of the aerosols. On the contrary, the activated fraction exhibits a strong correlation with the inferred critical diameter throughout the field campaigns. This suggests that the variability in the activated fraction is mostly driven by particle size, while variations in aerosol composition are of secondary importance. Moreover, our analysis suggests that the supersaturation reached in fog could be lowered by the aerosol number concentration, which could contribute to the sink term of water vapor during the radiative cooling. Although radiative fogs are usually associated with higher aerosol loading than stratus-lowering events, our analysis also reveals that the activated fraction at the beginning of the event is similar for both types of fog. However, the evolution of the droplet concentration during the fog life cycle shows significant differences between both types of fog. This work demonstrates that an accurate calculation of supersaturation is required to provide a realistic representation of fog microphysical properties in numerical models.

Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased hygroscopicity as well as diameter, facilitating droplet activation. This affects BC radiative forcing through aerosol-cloud interactions (aci) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015/16 in a residential area of Zurich which aimed at distinguishing different particle mixing states regarding hygroscopic properties in the cloud condensation nuclei (CCN)-activated fraction spectrum of urban aerosol and establishing relations between the mixing state of BC and its activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that, depending on the time of the day, we sampled both heavily aged internally mixed BC from background air advected to the site and freshly emitted externally mixed BC from local or regional traffic sources. During rush hours in the morning of weekdays, we found clear evidence that the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles which do not act as CCN within the CCNC. The mixing state of BC particles was also found to play a key role in their ability to form fog droplets. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have a very similar activation behavior as BC-free particles. The threshold coating thickness required for activation was shown to decrease with increasing BC core size. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core-shell particle geometry constrained with single particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size and mixing state resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.

Aerosol mass scattering efficiency affects climate forcing calculations, atmospheric visibility, and the interpretation of satellite observations of aerosol optical depth. We evaluated the representation of aerosol mass scattering efficiency (αsp) in the GEOS-Chem chemical transport model over North America using collocated measurements of aerosol scatter and mass from IMPROVE network sites between 2000 and 2010. We found a positive bias in mass scattering efficiency given current assumptions of aerosol size distributions and particle hygroscopicity in the model. We found that overestimation of mass scattering efficiency was most significant in dry (RH <35 %) and midrange humidity (35 % < RH <65 %) conditions, with biases of 82 % and 40 %, respectively. To address these biases, we investigated assumptions surrounding the two largest contributors to fine aerosol mass, organic (OA) and secondary inorganic aerosols (SIA). Inhibiting hygroscopic growth of SIA below 35 % RH and decreasing the dry geometric mean radius, from 0.069 µm for SIA and 0.073 µm for OA to 0.058 µm for both aerosol types, significantly decreased the overall bias observed at IMPROVE sites in dry conditions from 82 % to 9 %. Implementation of a widely used alternative representation of hygroscopic growth following κ-Kohler theory for secondary inorganic (hygroscopicity parameter κ=0.61) and organic (κ=0.10) aerosols eliminated the remaining overall bias in αsp. Incorporating these changes in aerosol size and hygroscopicity into the GEOS-Chem model resulted in an increase of 16 % in simulated annual average αsp over North America, with larger increases of 25 % to 45 % in northern regions with high RH and hygroscopic aerosol fractions, and decreases in αsp up to 15 % in the southwestern U.S. where RH is low.

Background and PurposeVirus-containing aerosol droplets emitted by breathing, speech or coughing dry rapidly to equilibrium with ambient relative humidity (RH), increasing in solute concentration with effects on virus survival and decreasing in diameter with effects on sedimentation and respiratory uptake. The aim of this paper is to model the effect of ionic and macromolecular solutes on droplet drying and solute concentration.MethodsDeliquescence-efflorescence concepts and Kohler theory were used to simulate the evolution of solute concentrations and water activity in respiratory droplets, starting from efflorescence data on mixed NaCl/KCl aerosols and osmotic pressure data on respiratory macromolecules.ResultsIn NaCl/KCl solutions supersaturated total salt concentrations were shown to reach 10-15M at the efflorescence RH of 40-55%, depending on the K:Na ratio. Dependence on K:Na ratio implies that the evaporation curves differ between aerosols derived from saliva and from airway surfaces. The direct effect of liquid droplet size through the Kelvin term was shown to be smaller and largely restricted to breath emissions. Modelling the effect of proteins and glycoproteins showed that salts determine drying equilibria down to the efflorescence RH, and macromolecules at lower RH.ConclusionDifferences in drying behaviour are predicted between breathing, speech and coughing emissions and between droplet size fractions within these. High salt concentrations may inactivate some viruses.

The activation of aerosol particles to form cloud droplets, a necessary first step in cloud formation, controls much of the impact that aerosols have on clouds and climate. Recently, there has been a surge of interest in extending the Kohler theory of cloud droplet activation to include surface active (typically organic) as well as water-soluble (typically inorganic) aerosol components, but a systematic framework for doing this has yet to be developed. Here, we apply a droplet stability analysis to this end. Ideal and Szyszkowski-Langmuir surfactant models are analyzed to demonstrate the new approach, but the underlying theoretical framework is fundamental and model free. A key finding is that superficial densities at the cloud activation threshold (Kohler maximum) are significantly sub-monolayer, with fractional coverage ranging from 69% to 85% for the organic compounds and mixtures studied. The result, significant for model inventories of cloud condensation nuclei, is a weakening of the surfactant effect relative to expectations based on bulk sample measurements. Analytical results are obtained for the loci of Kohler maxima and applied to aerosol mixtures containing an arbitrary number of water-soluble and surfactant components.

Secondary organic aerosol (SOA) is an important component of fine particular matter (PM2.5). Most air quality models use an equilibrium partitioning method along with the saturation vapor pressure (SVP) of semivolatile organic compounds (SVOCs) to predict SOA formation. However, the models typically assume that the organic particulate matter (OPM) is an ideal mixture and ignore the partitioning of water vapor to OPM. In this study, the Community Multiscale Air Quality model (CMAQ) is updated to investigate the impacts of water vapor partitioning and nonideality of the organic–water mixture on SOA formation during winter (January) and summer (July) of 2013 over eastern China. The updated model treats the partitioning of water vapor molecules into OPM and uses the universal functional activity coefficient (UNIFAC) model to estimate the activity coefficients of species in the organic–water mixture. The modified model can generally capture the observed surface organic carbon (OC) with a correlation coefficient R of 0.7 and the surface organic aerosol (OA) with the mean fractional bias (MFB) and mean fractional error (MFE) of −0.28 and 0.54, respectively. SOA concentration shows significant seasonal and spatial variations, with high concentrations in the North China Plain (NCP), central China, and the Sichuan Basin (SCB) regions during winter (up to 25 µg m−3) and in the Yangtze River Delta (YRD) during summer (up to 16 µg m−3). In winter, SOA decreases slightly in the updated model, with a monthly averaged relative change of 10 %–20 % in the highly concentrated areas, mainly due to organic–water interactions. The monthly averaged concentration of SOA increases greatly in summer, by 20 %–50 % at the surface and 30 %–60 % in the whole column. The increase in SOA is mainly due to the increase in biogenic SOA in inland areas and anthropogenic SOA in coastal areas. As a result, the averaged aerosol optical depth (AOD) is increased by up to 10 %, and the cooling effect of aerosol radiative forcing (ARF) is enhanced by up to 15 % over the YRD in summer. The aerosol liquid water content associated with OPM (ALWorg) at the surface is relatively high in inland areas in winter and over the ocean in summer, with a monthly averaged concentration of 0.5–3.0 and 5–7 µg m−3, respectively. The hygroscopicity parameter κ of OA based on the κ–Köhler theory is determined using the modeled ALWorg. The correlation of κ with the O:C ratio varies significantly across different cities and seasons. Analysis of two representative cities, Jinan (in the NCP) and Nanjing (in the YRD), shows that the impacts of water partitioning and nonideality of the organic–water mixture on SOA are sensitive to temperature, relative humidity (RH), and the SVP of SVOCs. The two processes exhibit opposite impacts on SOA in eastern China. Water uptake increases SOA by up to 80 % in the organic phase, while including nonunity activity coefficients decreases SOA by up to 50 %. Our results indicate that both water partitioning into OPM and the activity coefficients of the condensed organics should be considered in simulating SOA formation from gas–particle partitioning, especially in hot and humid environments.

The physical processes and time scales underlying the evolution of surface tension in atmospheric solution droplets are largely unaccounted for in present models describing cloud droplet formation. Adsorption of surface-active molecules at the surface of a solution droplet depresses the droplet surface tension but also depletes solute from the droplet bulk, which have opposing and sometimes canceling effects in cloud droplet formation. In this work, we study the effect of time-evolving surface tension for cloud droplet activation of particles composed of Nordic Aquatic Fulvic Acid (NAFA) mixed with sodium chloride (NaCl). We model the formation of cloud droplets using Köhler theory with surface tension depression and bulk/surface partitioning evaluated from two different thermodynamic surface models. Continuous ternary parameterizations were constructed from surface tension measurements of macroscopic droplets at different time steps after the formation of a droplet surface. The predicted results are compared to previous measurements of mixed NAFA-NaCl cloud condensation nuclei (CCN) activity and a bulk solution model that does not take the NAFA bulk/surface partitioning equilibrium into account. Whereas the bulk model shows a trend in cloud droplet formation following that of macroscopic surface tension depression with time, the variation with time essentially disappears when bulk/surface partitioning is taken explicitly into account during droplet activation. For all equilibrium time steps considered, the effect of surface tension depression in the NAFA-NaCl system is counteracted by the depletion of solute from the finite-sized droplet bulk phase. Our study highlights that a comprehensive data set is necessary to obtain continuous parameterizations of surface tension and other solution properties required to fully account for the bulk/surface partitioning in growing droplets. To our knowledge, no similar data set currently exists for other aqueous organic systems of atmospheric interest. Additional work is necessary to deconvolve the effects of bulk/surface partitioning in the context of time-evolution on cloud droplet activation and to determine whether the results presented here can be further generalized.

Hygroscopicity measurements of secondary organic aerosol (SOA) particles often show inconsistent results between the supersaturated and subsaturated regimes, with higher activity as cloud condensation nucleus (CCN) than indicated by hygroscopic growth. In this study, we have investigated the discrepancy between the two regimes in the Lund University (LU) smog chamber. Various anthropogenic SOA were produced from mixtures of different precursors: anthropogenic light aromatic precursors (toluene and m-xylene), exhaust from a diesel passenger vehicle spiked with the light aromatic precursors, and exhaust from two different gasoline-powered passenger vehicles. Three types of seed particles were used: soot aggregates from a diesel vehicle, soot aggregates from a flame soot generator and ammonium sulphate (AS) particles. The hygroscopicity of seed particles with condensed, photochemically produced, anthropogenic SOA was investigated with respect to critical supersaturation (sc) and hygroscopic growth factor (gf) at 90% relative humidity. The hygroscopicity parameter κ was calculated for the two regimes: κsc and κgf, from measurements of sc and gf, respectively. The two κ showed significant discrepancies, with a κgf /κsc ratio closest to one for the gasoline experiments with ammonium sulphate seed and lower for the soot seed experiments. Empirical observations of sc and gf were compared to theoretical predictions, using modified Kohler theory where water solubility limitations were taken into account. The results indicate that the inconsistency between measurements in the subsaturated and supersaturated regimes may be explained by part of the organic material in the particles produced from anthropogenic precursors having a limited solubility in water.

Cooking organic aerosol (COA) is potentially a significant fraction of organic particulate matter in urban areas. COA chemical aging experiments, using aerosol produced by grilling hamburgers, took place in a smog chamber in the presence of UV light or excess ozone. The water solubility distributions, cloud condensation nuclei (CCN) activity, and corresponding hygroscopicity of fresh and aged COA were measured. The average mobility equivalent activation diameter of the fresh particles at 0.4% supersaturation ranged from 87 to 126 nm and decreased for aged particles, ranging from 65 to 88 nm. Most of the fresh COA had water solubility less than 0.1 g L−1, even though the corresponding particles were quite CCN active. After aging, the COA fraction with water solubility greater than 0.1 g L−1 increased more than 2 times. Using the extended Kohler theory for multiple partially soluble components in order to predict the measured activation diameters, the COA solubility distribution alone could not explain the CCN activity. Surface tensions less than 30 dyn cm−1 were required to explain the measured activation diameters. In addition, COA particles appear to not be spherical, which can introduce uncertainties into the corresponding calculations.

Bidirectional fog droplet fluxes were observed at two mountainous subtropical forests in East Asia. To investigate the various boundary conditions and that cause these bidirectional droplet fluxes, we set up identical eddy covariance systems including a droplet spectrometer (FM100 Fog monitor) at two study sites in the Ailaoshan (SW China) and Xitou (central Taiwan) areas for several weeks in winter 2015/2016 and spring 2017, respectively. Normally, fog droplets are expected to have a downward flux toward the surface for all sizes due to impaction at the vegetation’s surface. However, we also observed temporally positive fluxes, for fog droplets up to a diameter of 10 μm. Two different cases of bidirectional fog droplet fluxes were identified in our experiments: At Xitou, the positive droplet number fluxes for smaller droplets occurred together with a positive sensible heat flux in combination with large critical diameters according to the Kohler theory. At Ailaoshan, similar fluxes occurred yet together with negative sensible heat fluxes in combination with small critical diameters. We analyze the occurrence of these bidirectional droplet number fluxes in conjunction with the boundary layer conditions and the activation state of the droplets with diameters up to 10 μm. Plausible reasons for the identical flux directions at the two sites under very different microphysical fog conditions are presented.

To investigate interactions between aerosols and clouds, the size and number concentrations of the cloud condensation nuclei (CCN) and the cloud droplets (CDs) were measured at the summit of Mt. Fuji (altitude 3776 m), Japan. The CCN number concentrations (NCCN) are significantly higher in continental air masses than in air masses from the Pacific Ocean. The hygroscopicity parameter κ did not change much for different air mass origins, indicating that aerosol particles in the free troposphere are well mixed. Based on the CD number concentrations (NCD), the degree of supersaturation in the ambient air during the cloud-shrouded period was estimated to be 0.15% (25th percentile) to 0.44% (75th percentile). To evaluate factors influencing the NCD, measured NCD were compared to ones calculated based on the Köhler theory using aerosol number size distributions, κ, and the degree of supersaturation. The results showed that NCD could not be reproduced satisfyingly when the mean number size distribution or the mean effective supersaturation were used for the calculation. This study highlights the importance of obtaining information about the degree of supersaturation to predict NCD in the atmosphere.

Capillary condensation (CC), namely, the formation from the vapor of a stable phase of drops below the saturation pressure, is a prevalent phenomenon. It may occur inside porous structures or between surfaces of particles. CC between surfaces, a liquid "bridge", is of particular practical interest because of its resulting adhesive force. To date, studies have focused on pure water condensation. However, nonvolatile materials, such as salts and surfactants, are prevalent in many environments. In the current study, the effect of these contaminants on CC is investigated from a thermodynamic point of view. This is done by computing the Gibbs energy of such systems and developing the modified Kelvin equation, based on the Kohler theory. The results demonstrate that nonvolatile solutes may have a number of major effects, including an increase in the critical radius and the stabilization of the newly formed phase.

Number concentration measurements of cloud condensation nuclei (CCN) at five supersaturation values between 0.2 and 1.0% were made from a coastal site (Thiruvananthapuram) of peninsular India using a single column CCN counter during the summer monsoon period (June–September) of 2013 and 2014. The CCN concentration over this site showed diurnal variations of high values during nighttime and low values during daytime in association with the change in mesoscale circulation patterns. The inter-annual variations of CCN (CCN 0.4% = 2,232 ± 672 cm −3 during August 2013 and CCN 0.4% = 941 ± 325 cm −3 during August 2014) are mostly associated with the varying intensity of monsoon rainfall. The variation of CCN number concentration with supersaturation is found to be steeper during nighttime (indicating a less CCN active aerosol system) than during daytime (CCN active system). The CCN activation ratio estimated using simultaneous measurements of CCN and aerosol number (CN) concentration clearly depict the role of land-sea breeze circulations with higher values during daytime than the nighttime. The CCN number concentration predicted for different supersaturations, from measured aerosol number size distribution using Kohler theory, indicate the importance of the change in aerosol composition associated with different airmasses in a coastal environment.

The albedo and microphysical properties of clouds are controlled in part by the hygroscopicity of particles serving as cloud condensation nuclei (CCN). Hygroscopicity of complex organic mixtures in the atmosphere varies widely and remains challenging to predict. Here we present new measurements characterizing the CCN activity of pure compounds in which carbon chain length and the numbers of hydroperoxy, carboxyl, and carbonyl functional groups were systematically varied to establish the contributions of these groups to organic aerosol apparent hygroscopicity. Apparent hygroscopicity decreased with carbon chain length and increased with polar functional groups in the order carboxyl > hydroperoxy > carbonyl. Activation diameters at different supersaturations deviated from the -3/2 slope in log-log space predicted by Kohler theory, suggesting that water solubility limits CCN activity of particles composed of weakly functionalized organic compounds. Results are compared to a functional group contribution model that predicts CCN activity of organic compounds. The model performed well for most compounds but underpredicted the CCN activity of hydroperoxy groups. New best-fit hydroperoxy group/water interaction parameters were derived from the available CCN data. These results may help improve estimates of the CCN activity of ambient organic aerosols from composition data.

The cloud condensation nuclei (CCN) closure study was performed to exemplify the effect of aerosol chemical composition on the CCN activity of aerosols at Mahabaleshwar, a high altitude background site in the Western Ghats, India. For this, collocated aerosol, CCN, Elemental Carbon (EC), Organic Carbon (OC), sub-micron aerosol chemical speciation for the period from 3rd June to 19th June 2015 was used. The chemical composition of non-refractory particulate matter ( −3 for organics, ammonium, chloride, nitrate and sulphate, respectively. The PM 1 number concentration as obtained by Wide Range Aerosol Spectrometer (WRAS) varied from 750 to 6480 cm −3 . The average mass concentration of elemental carbon (EC) as measured by OC-EC analyzer was 1.16 ± 0.4 μg m −3 . The average CCN concentrations obtained from CCN counter (CCNC) at five super-saturations (SS's) was 118 ± 58 cm −3 (0.1% SS), 873 ± 448 cm −3 (0.31% SS), 1308 ± 603 cm −3 (0.52% SS), 1610 ± 838 cm −3 (0.73% SS) and 1826 ± 985 cm −3 (0.94% SS). The CCN concentrations were predicted using Kohler theory on the basis of measured aerosol particle number size distribution, size independent NR-PM1 chemical composition and calculated hygroscopicity. The CCN closure study was evaluated for 3 scenarios, B-I (all soluble inorganics), B-IO (all soluble organics and inorganics) and B-IOOA (all soluble inorganic and soluble oxygenated organic aerosol, OOA). OOA component was derived from the positive matrix factorization (PMF) analysis of organic aerosol mass spectra. Considering the bulk composition as internal mixture, CCN closure study was underestimated by 16–39% for B-I and overestimated by 47–62% for B-IO. The CCN closure result was appreciably improved for B-IOOA where the knowledge of OOA fraction was introduced and uncertainty reduced to within 8–10%.

The spontaneous growth of cloud condensation nuclei (CCN) into cloud droplets under supersaturated water vapour conditions is described by classic Kohler theory(1,2). This spontaneous activation of CCN depends on the interplay between the Raoult effect, whereby activation potential increases with decreasing water activity or increasing solute concentration, and the Kelvin effect, whereby activation potential decreases with decreasing droplet size or increases with decreasing surface tension, which is sensitive to surfactants(1). Surface tension lowering caused by organic surfactants, which diminishes the Kelvin effect, is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of surfactant molecules from the droplet bulk to the droplet-vapour interface(3,4). Here we present observational and theoretical evidence illustrating that, in ambient air, surface tension lowering can prevail over the reduction in the Raoult effect, leading to substantial increases in cloud droplet concentrations. We suggest that consideration of liquid-liquid phase separation, leading to complete or partial engulfing of a hygroscopic particle core by a hydrophobic organic-rich phase, can explain the lack of concomitant reduction of the Raoult effect, while maintaining substantial lowering of surface tension, even for partial surface coverage. Apart from the importance of particle size and composition in droplet activation, we show by observation and modelling that incorporation of phase-separation effects into activation thermodynamics can lead to a CCN number concentration that is up to ten times what is predicted by climate models, changing the properties of clouds. An adequate representation of the CCN activation process is essential to the prediction of clouds in climate models, and given the effect of clouds on the Earth's energy balance, improved prediction of aerosol-cloud-climate interactions is likely to result in improved assessments of future climate change.

Changes in aerosol chemical mixtures modify cloud condensation nuclei (CCN) activity. Previous studies have developed CCN models and validated changes in external and internal mixing state with ambient field data. Here, we develop an experimental method to test and validate the CCN activation of known aerosol chemical composition with multicomponent mixtures and varying mixing states. CCN activation curves consisting of one or more activation points are presented. Specifically, simplified two-component systems of varying hygroscopicity were generated under internal, external, and transitional mixing conditions. κ-Köhler theory predictions were calculated for different organic and inorganic mixtures and compared to experimentally derived kappa values and respective mixing states. This work employs novel experimental methods to provide information on the shifts in CCN activation data due to external to internal particle mixing from controlled laboratory sources. Results show that activation curves consisting of single and double activation points are consistent with internal and external mixtures, respectively. In addition, the height of the plateau at the activation points is reflective of the externally mixed concentration in the mixture. The presence of a plateau indicates that CCN activation curves consisting of multiple inflection points are externally mixed aerosols of varying water-uptake properties. The plateau disappears when mixing is promoted in the flow tube. At the end of the flow tube experiment, the aerosols are internally mixed and the CCN activated fraction data can be fit with a single-sigmoid curve. The technique to mimic externally to internally mixed aerosol is applied to non-hygroscopic carbonaceous aerosol with organic and inorganic components. To our knowledge, this work is the first to show controlled CCN activation of mixed non-hygroscopic soot with hygroscopic material as the aerosol population transitions from externally to internally mixed states in laboratory conditions. Results confirm that CCN activation analysis methods used here and in ambient data sets are robust and may be used to infer the mixing state of complex aerosol compositions of unknown origin.

Aerosol liquid water (ALW) is ubiquitous in ambient aerosol and plays an important role in the formation of both aerosol organics and inorganics. To investigate the interactions between ALW and aerosol organics during haze formation and evolution, ALW was modelled based on long-term measurement of submicron aerosol composition in different seasons in Beijing. ALW contributed by aerosol inorganics (ALWinorg) was modelled by ISORROPIA II, and ALW contributed by organics (ALWorg) was estimated with κ-Köhler theory, where the real-time hygroscopicity parameter of the organics (κorg) was calculated from the real-time organic oxygen-to-carbon ratio (O∕C). Overall particle hygroscopicity (κtotal) was computed by weighting component hygroscopicity parameters based on their volume fractions in the mixture. We found that ALWorg, which is often neglected in traditional ALW modelling, contributes a significant fraction (18 %–32 %) to the total ALW in Beijing. The ALWorg fraction is largest on the cleanest days when both the organic fraction and κorg are relatively high. The large variation in O∕C, from 0.2 to 1.3, indicates the wide variety of organic components. This emphasizes the necessity of using real-time κorg, instead of fixed κorg, to calculate ALWorg in Beijing. The significant variation in κorg (calculated from O∕C), together with highly variable organic or inorganic volume fractions, leads to a wide range of κtotal (between 0.20 and 0.45), which has a great impact on water uptake. The variation in organic O∕C, or derived κorg, was found to be influenced by temperature (T), ALW, and aerosol mass concentrations, among which T and ALW both have promoting effects on O∕C. During high-ALW haze episodes, although the organic fraction decreases rapidly, O∕C and derived κorg increase with the increase in ALW, suggesting the formation of more soluble organics via heterogeneous uptake or aqueous processes. A positive feedback loop is thus formed: during high-ALW episodes, increasing κorg, together with decreasing particle organic fraction (or increasing particle inorganic fraction), increases κtotal, and thus further promotes the ability of particles to uptake water.

Large-Eddy Simulations (LES) are an excellent tool to improve our understanding of the aerosol-cloud interaction (ACI). These models combine a spatial resolution high enough to resolve cloud structures with domain sizes large enough to simulate macroscale dynamics and feedback between clouds. However, most research on ACI using LES simulations is focused on changes in cloud characteristics. The feedback of ACI on the aerosol population remains relatively understudied. We introduce a prognostic aerosol scheme with multiple aerosol species in the Dutch Atmospheric Large-Eddy Simulation model (DALES), especially focused on simulating the feedback of ACI on the aerosol population. The numerical treatment of aerosol activation is a crucial element in the simulation of ACI. Two methods are implemented and discussed: an explicit activation scheme based on κ-Köhler theory and a more classic approach using updraft strength. Model simulations are validated against observations using the Rain in Shallow Cumulus over the Ocean (RICO) campaign, characterised by rapidly precipitating, warm-phase shallow cumulus clouds. We find that in this pristine ocean environment virtually all aerosols enter the cloud phase through activation while in-cloud scavenging is relatively inefficient. Despite the rapid formation of precipitation, most of the in-cloud aerosol mass is returned to the atmosphere by cloud evaporation. The strength of aerosol processing through subsequent cloud cycles is found to be particularly sensitive to the activation scheme and resulting cloud characteristics. However, the precipitation processes are considerably less sensitive. Scavenging by precipitation is the dominant source for in-rain aerosol mass. About half of the in-rain aerosol reaches the surface, while the rest is released by evaporation of falling precipitation. Whether ACI increases or decreases the average aerosol size depends on the balance between the evaporation of clouds and rain, and ultimate removal by precipitation. Analysis of typical aerosol size associated with the different microphysical processes shows that aerosols resuspended by cloud evaporation are only 5 to 10 % larger than the originally activated aerosols. In contrast, aerosols released by evaporating precipitation are an order of magnitude larger.

Liquid clouds form by condensation of water vapour on aerosol particles in the atmosphere. Even black carbon (BC) particles, which are known to be slightly hygroscopic, have been shown to readily form cloud droplets once they have acquired water-soluble coatings by atmospheric aging processes. Accurately simulating the life cycle of BC in the atmosphere, which strongly depends on the wet removal following droplet activation, has recently been identified as a key element for accurate prediction of the climate forcing of BC. Here, to assess BC activation in detail, we performed in situ measurements during cloud events at the Jungfraujoch high-altitude station in Switzerland in summer 2010 and 2016. Cloud droplet residual and interstitial (unactivated) particles as well as the total aerosol were selectively sampled using different inlets, followed by their physical characterization using scanning mobility particle sizers (SMPSs), multi-angle absorption photometers (MAAPs) and a single-particle soot photometer (SP2). By calculating cloud droplet activated fractions with these measurements, we determined the roles of various parameters on the droplet activation of BC. The half-rise threshold diameter for droplet activation (Dhalfcloud), i.e. the size above which aerosol particles formed cloud droplets, was inferred from the aerosol size distributions measured behind the different inlets. The effective peak supersaturation (SSpeak) of a cloud was derived from Dhalfcloud by comparing it to the supersaturation dependence of the threshold diameter for cloud condensation nuclei (CCN) activation measured by a CCN counter (CCNC). In this way, we showed that the mass-based scavenged fraction of BC strongly correlates with that of the entire aerosol population because SSpeak modulates the critical size for activation of either particle type. A total of 50 % of the BC-containing particles with a BC mass equivalent core diameter of 90 nm was activated in clouds with SSpeak≈0.21 %, increasing up to ∼80 % activated fraction at SSpeak≈0.50 %. On a single-particle basis, BC activation at a certain SSpeak is controlled by the BC core size and internally mixed coating, which increases overall particle size and hygroscopicity. However, the resulting effect on the population averaged and on the size-integrated BC scavenged fraction by mass is small for two reasons: first, acquisition of coatings only matters for small cores in clouds with low SSpeak; and, second, variations in BC core size distribution and mean coating thickness are limited in the lower free troposphere in summer. Finally, we tested the ability of a simplified theoretical model, which combines the κ-Köhler theory with the Zdanovskii–Stokes–Robinson (ZSR) mixing rule under the assumptions of spherical core–shell particle geometry and surface tension of pure water, to predict the droplet activation behaviour of BC-containing particles in real clouds. Predictions of BC activation constrained with SSpeak and measured BC-containing particle size and mixing state were compared with direct cloud observations. These predictions achieved closure with the measurements for the particle size ranges accessible to our instrumentation, that is, BC core diameters and total particle diameters of approximately 50 and 180 nm, respectively. This clearly indicates that such simplified theoretical models provide a sufficient description of BC activation in clouds, as previously shown for activation occurring in fog at lower supersaturation and also shown in laboratory experiments under controlled conditions. This further justifies application of such simplified theoretical approaches in regional and global simulations of BC activation in clouds, which include aerosol modules that explicitly simulate BC-containing particle size and mixing state.

The ability of a particle to uptake water and form a cloud droplet depends on its hygroscopicity. To understand its impact on cloud properties and ultimately radiative forcing, knowledge of chemically-resolved mixing state information or the one based on hygroscopic growth is crucial. Typically, global models assume either pure internal or external mixing state which might not be true for all conditions and sampling locations. To investigate into this, the current study employed an indirect approach to infer the probable mixing state. The hygroscopic parameters derived from κ -Kohler theory using size-resolved CCN measurements ( κ CCN ) and bulk/size-resolved aerosol mass spectrometer (AMS) measurements ( κ AMS ) were compared. The accumulation mode particles were found to be more hygroscopic ( κ CCN = 0.24) than Aitken mode ( κ CCN = 0.13), perhaps due to increased ratio of inorganic to organic mass fraction. The activation diameter calculated from size-resolved CCN activity measurements at 5 different supersaturation (SS) levels varied in the range of 115 nm–42 nm with κ CCN = 0.13–0.23 (avg = 0.18 ± 0.10 (±1σ)). Further, κ AMS > κ CCN was observed possibly due to the fact that organic and inorganic mass present in the Aitken mode was not correctly represented by bulk chemical composition and size-resolved fractional contribution of oxidized OA was not accurately accounted. Better correlation of organic fraction (f org ) and κ CCN at lower SS explained this behaviour. The decrease in κ CCN with the time of the day was more pronounced at lower SS because of the relative mass reduction of soluble inorganic species by ∼17%. Despite the large differences between κ measured from two approaches, less over-prediction (up to 18%) between measured and predicted CCN concentration suggested lower impact of chemical composition and mixing state at higher SS. However, at lower SS, presences of externally mixed CCN-inactive aerosols lead to CCN over-prediction reflecting the significance of aerosol mixing state information. Further examination of the effect of biomass burning aerosols (∼35% in least oxidized biomass burning organic aerosol (BBOA-2 fraction) on hygroscopicity and CCN activity showed increase in the concentration of all AMS measured species (except NH 4 + and SO 4 2− ), less O:C ratio, and organic mass fraction (f org ) peak shift to lower diameter range caused ∼13% change in critical diameter (D a ) and ∼40% change in κ CCN . Increased deviation of ∼100% between κ CCN and κ AMS due to sudden influx of internally mixed BBOA caused suppressed hygroscopic growth. This study finally suggests the assumption of pure internally mixed aerosol does not completely hold true for this anthropogenically polluted site.

Microphysical processes of fog and their spatial and temporal pattern are a challenge to study under natural conditions. This work focuses on the development of bidirectional fluxes of fog droplets above a forest canopy in northeastern Taiwan. Bidirectional fluxes occurred regularly, start from the smallest droplet class (

This work presents experimental data on the cloud condensation nuclei (CCN) activity of two-component mixtures containing surfactants. Nine binary systems were tested combining strong ionic (sodium dodecyl sulfate) and nonionic surfactants (Zonyl FS-300 and Triton X-100) with nonsurfactant compounds (glucose, ammonium sulfate, or sodium chloride). Control tests were performed for systems combining organic (glucose) and inorganic compounds (ammonium sulfate or sodium chloride). Results show that CCN activity deviates strongly relative to predictions made from measurements of bulk surface tension. Kohler theory accounting for surface tension reduction and surface partitioning underpredicts the CCN activity of particles containing Zonyl FS-300 and Triton X-100. Partitioning theory better describes data for Zonyl FS-300 and Triton X-100 when limiting surface adsorption to 1.5 monolayers of the growing drop. Deviations from predictions were observed. Likely explanations include solute-solute interactions and nonspherical particle shape. The findings presented here examine in detail the perturbation of CCN activity by surfactants and may offer insight into both the success and limitations of physical models describing CCN activity of surface active molecules.

Radioactive aerosol released under severe nuclear accidents conditions contains large amounts of soluble compounds. The hygroscopic growth of soluble aerosol enable to enlarge the particle size and affect the subsequent deposition behavior, which plays an important role on source term analysis. However, the investigation about hygroscopic growth properties of typical nuclear aerosol viz. Cesium iodine and cesium hydroxide, has been largely lacking and the hygroscopic model in MELCOR also need to validate and evaluate. In this paper, steady-state hygroscopic model based on Kohler theory was used to predict the hygroscopic growth factors of these two kinds of aerosols. Sensitivity analysis of surface tension and water activity of aqueous-solution droplet on hygroscopic growth factor were performed, and the prediction results were compared with the experimental data to evaluate MELCOR. The results show that the simplification of replacing surface tension of salt droplet with pure water in MELCOR is acceptable. The processing method of water activity in MELCOR overestimates the hygroscopic growth factors of cesium hydroxide, while its predictions are much close to the hygroscopic growth factors of cesium iodine. The improved model has higher prediction accuracy than MELCOR. In addition, the transient hygroscopic growth rate model was also used to analyze the effects of operating parameters on the hygroscopic growth characteristics of soluble aerosol. The hygroscopic growth rate is proportional to the relative humidity, particle size and gas temperature. Aerosol particles with larger initial size under higher relative humidity condition require longer time to attain equilibrium state, and the equilibrium time decreases with the increasing gas temperature. This study can provide theoretical reference for fundamental understanding of hygroscopic growth properties of soluble aerosol and the estimation of aerosol source terms under severe nuclear accidents conditions.

Calculating the equilibrium composition of atmospheric aerosol particles, using all variations of Köhler theory, has largely assumed that the total solute concentrations define both the water activity and surface tension. Recently however, bulk to surface phase partitioning has been postulated as a process which significantly alters the predicted point of activation. In this paper, an analytical solution to calculate the removal of material from a bulk to a surface layer in aerosol particles has been derived using a well established and validated surface tension framework. The applicability to an unlimited number of components is possible via reliance on data from each binary system. Whilst assumptions regarding behaviour at the surface layer have been made to facilitate derivation, it is proposed that the framework presented can capture the overall impact of bulk-surface partitioning. Demonstrations of the equations for two and five component mixtures are given while comparisons are made with more detailed frameworks capable at modelling ternary systems at higher levels of complexity. Predictions made by the model across a range of surface active properties should be tested against measurements. Indeed, reccomendations are given for experimental validation and to assess sensitivities to accuracy and required level of complexity within large scale frameworks. Importantly, the computational efficiency of using the solution presented in this paper is roughly a factor of 20 less than a similar iterative approach, a comparison with highly coupled approaches not available beyond a 3 component system.

New particle formation involving sulfuric acid, bases and oxidized organic compounds is an important source of atmospheric aerosol particles. One of the mechanisms suggested to depict this process is the nano-Köhler theory, which describes the activation of inorganic molecular clusters to growth by a soluble organic vapor. In this work we studied the capability of the nano-Köhler theory to describe the growth of atmospheric molecular clusters by simulating the dynamics of a cluster population in the presence of a sulfuric acid–base mixture and an organic compound. We observed nano-Köhler type activation in our simulations when the saturation ratio of the organic vapor and the ratio between organic and inorganic vapor concentrations were in a suitable range. However, the nano-Köhler theory was unable to predict the exact size at which the activation occurred in the simulations. In some conditions apparent cluster growth rate (GR) started to increase close to the activation size determined from the simulations. Nevertheless, because the behavior of GR is also affected by other dynamic processes, GR alone cannot be used to deduce the cluster growth mechanism.

Aerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set - ready to be used for model validation - of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles 20nm) across the range of 0.1 to 1.0% supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2-0.3). We performed closure studies based on -Kohler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of . The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating migrating-CCNCs to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved. © Author(s) 2018. This work is distributed under the Creative Commons Attribution 4.0 License.