Cloud Condensation Nuclei Counter Research Articles

A New Method for Size‐Resolved Aerosol CCN Activity Measurement at Low Supersaturation in Pristine Atmosphere

AbstractUnderstanding aerosol‐cloud interactions under pristine atmospheric conditions is crucial for meaningful global climate change predictions. However, ability of aerosol particles to act as cloud condensation nuclei (CCN) activity of aerosols in pristine atmosphere remains limited, mainly because of the difficulty of measuring it in pristine environments. Given the extremely low CCN number concentration under low supersaturations (SSs) and the complex impact of the kinetic limitation in CCN measurements, size‐resolved CCN activity measurements at low SSs cannot be achieved with traditional methods using differential mobility analyzers and a CCN counter (CCNC) because of the low sample efficiency and the impact of particles with multiple charges. To overcome this difficulty, we propose a new method for measuring size‐resolved CCN activity at low aerosol number concentrations. The new method is based on a combined system comprising an aerodynamic aerosol classifier (AAC) and a CCNC (AAC‐CCNC system). A control program was developed to achieve high‐resolution scans of the SS and particle size within a reasonable time frame. A data inversion scheme, including corrections for the transfer function and kinetic limitation, was developed to obtain accurate size‐resolved CCN activity. In July‐August 2022, the new method was used to measure the size‐resolved CCN activity on the Tibetan Plateau. This new method can advance the size‐resolved CCN measurements, thereby enhancing our understanding of aerosol‐cloud interactions in pristine atmosphere.

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E–150°E) During the Spring and Summer: Results From MARCUS (I)

AbstractThe Atmospheric Radiation Measurement Mobile Facility‐2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017–2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60°S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra‐High‐Sensitivity Aerosol Spectrometer show that both the number concentration (NCCN) and size distribution of CCN‐active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50°S–60°S) and the South Southern Ocean (SSO) (62°S–68°S). The average NSO NCCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat‐labile and presumably proteinacous INPs suggests an increase of ice nucleating‐active microbes in summer.

A remote sensing algorithm for vertically resolved cloud condensation nuclei number concentrations from airborne and spaceborne lidar observations

Abstract. Cloud condensation nuclei (CCN) are mediators of aerosol–cloud interactions (ACIs), contributing to the largest uncertainties in the understandings of global climate change. We present a novel remote-sensing-based algorithm that quantifies the vertically resolved CCN number concentrations (NCCN) using aerosol optical properties measured by a multiwavelength lidar. The algorithm considers five distinct aerosol subtypes with bimodal size distributions. The inversion used the lookup tables developed in this study, based on the observations from the Aerosol Robotic Network, to efficiently retrieve optimal particle size distributions from lidar measurements. The method derives dry aerosol optical properties by implementing hygroscopic enhancement factors in lidar measurements. The retrieved optically equivalent particle size distributions and aerosol-type-dependent particle composition are utilized to calculate critical diameters using κ-Köhler theory and NCCN at six supersaturations ranging from 0.07 % to 1.0 %. Sensitivity analyses indicate that uncertainties in extinction coefficients and relative humidity greatly influence the retrieval error in NCCN. The potential of this algorithm is further evaluated by retrieving NCCN using airborne lidar from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) campaign and is validated against simultaneous measurements from the CCN counter. The independent validation with robust correlation demonstrates promising results. Furthermore, the NCCN has been retrieved for the first time using a proposed algorithm from spaceborne lidar – Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) – measurements. The application of this new capability demonstrates the potential for constructing a 3D CCN climatology at a global scale, which helps to better quantify ACI effects and thus reduce the uncertainty in aerosol climate forcing.

On the correlation between hygroscopic properties and chemical composition of cloud condensation nuclei obtained from the chemical aging of soot particles with O3 and SO2

Soot particles released in the atmosphere have long been investigated for their ability to affect the radiative forcing. Although freshly emitted soot particles are generally considered to yield only positive contributions to the radiative forcing, atmospheric aging can activate them into efficient cloud condensation or ice nuclei, which can trigger the formation of persistent clouds and ultimately provide a negative contribution to the radiative forcing. Depending on their residence time in the atmosphere, soot particles can undergo several physical and chemical aging processes that affect their chemical composition, particle size distribution and morphology, and ultimately their optical and hygroscopic properties. The impact of the physical-chemical aging on the properties of soot particles is still difficult to quantify, as well as their effect on the radiative forcing of the atmosphere.This work investigates the hygroscopic properties of chemically aged soot particles obtained from the combustion of aviation fuel, and in particular the interplay between aging mechanisms initiated by two widespread atmospheric oxidizers (O3 and SO2). Activation is measured in water supersaturation conditions using a cloud condensation nuclei counter. Once particle morphology and size distribution are taken into account, the hygroscopicity parameter κ is derived using κ-Köhler theory and correlated to the change of the chemical composition of the particles aged in a simulation chamber. While fresh soot particles are poor cloud condensation nuclei (κ < 10−4) and are not significantly affected by either O3 or SO2 at the timescale of the experiments, rapid activation is observed when they are simultaneously exposed to both oxidizers. Activated particles become efficient cloud condensation nuclei, comparable to the highly hygroscopic particulate matter typically found in the atmosphere (κ = 0.2–0.6 at RH = 20 %). Statistical analysis reveals a correlation between the activation and sulfur-containing ions detected on the chemically aged particles that are absent from the fresh particles.

Cloud condensation nuclei activity of internally mixed particle populations at a remote marine free troposphere site in the North Atlantic Ocean

This study reports results from research conducted at the Observatory of Mount Pico (OMP), 2225 m above mean sea level on Pico Island in the Azores archipelago in June and July 2017. We investigated the chemical composition, mixing state, and cloud condensation nuclei (CCN) activities of long-range transported free tropospheric (FT) particles. FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) simulations reveal that most air masses that arrived at the OMP during the sampling period originated in North America and were highly aged (average plume age > 10 days). We probed size-resolved chemical composition, mixing state, and hygroscopicity parameter (κ) of individual particles using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX). Based on the estimated individual particle mass from elemental composition, we calculated the mixing state index, χ. During our study, FT particle populations were internally mixed (χ of samples are between 53 % and 87 %), owing to the long atmospheric aging time. We used data from a miniature Cloud Condensation Nucleus Counter (miniCCNC) to derive the hygroscopicity parameter, κCCNC. Combining κCCNC and FLEXPART, we found that air masses recirculated above the North Atlantic Ocean with lower mean altitude had higher κCCNC due to the higher contribution of sea salt particles. We used CCSEM-EDX and phase state measurements to predict single-particle κ (κCCSEM-EDX) values, which overlap with the lower range of κCCNC measured below 0.15 % SS. Therefore, CCSEM-EDX measurements can be useful in predicting the lower bound of κ, which can be used in climate models to predict CCN activities, especially in remote locations where online CCN measurements are unavailable.

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

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

Investigating the Applicability of a Global Average Calibration Line for Ambient Size-Resolved Cloud Condensation Nuclei (CCN) Measurements: A Technical Note

Abstract Aerosol–cloud–precipitation interaction represents the largest uncertainty in climate change’s current and future understanding. Therefore, aerosol properties affecting the cloud and precipitation formation and their accurate estimation is a first step in developing improved parameterizations for the prognostic climate models. Over the last couple of decades, a commercially available Cloud Condensation Nuclei Counter (CCNC) has been deployed in the field and laboratory for characterizing CCN properties of ambient or atmospherically relevant laboratory-generated aerosols. However, most of the CCN measurements performed in the field are often compounded with the erroneous estimation of CCN concentration and other parameters due to a lack of robust and accurate CCNC calibration. CCNC is not a plug-and-play instrument and requires prudent calibration and operation, to avoid erroneous data and added parameterization uncertainties. In this work, we propose and demonstrate the usability of a global calibration equation derived from CCNC calibration experiments from 8 contrasting global environments. Significant correlation was observed between the global calibration and each of the 16 individual experiments. A significant improvement in the correlation was observed when the calibration experiments were separated for high-altitude measurements. Using these equations, we further derived the effective hygroscopicity parameter and found lower relative uncertainty in the hygroscopicity parameter at higher effective supersaturation. Our results signify that altitude-based pressure change could be of importance for accurate calibration at high-altitude locations. Our results are consistent with previous studies emphasizing the criticality of the accurate CCN calibration for the lower supersaturations.

The hygroscopic properties of biomass burning aerosol from Eucalyptus and cow dung under different combustion conditions

Aerosols hygroscopic growth is of current interest due to its effect on atmospheric light scattering and extinction. Knowledge of hygroscopic properties is essential for predicting the effect of aerosol on cloud formation, regional visibility, climate impact, and lung deposition. Previous studies have used surrogate components of complex aerosol; and the application to complex multi-component aerosol like biomass burning aerosol is limited. We report aerosol hygroscopicity parameter of biomass burning aerosol derived from Eucalyptus and cow dung in a humidified smog chamber using two techniques: (1) measuring extinction hygroscopic enhancement factor f(RH) of aerosol using a cavity ring down spectrometer and deriving the hygroscopicity parameter using empirical equations and (2) directly using a Cloud Condensation Nuclei Counter (CCNC). Based on repeated measurements of the same fuel under different burning conditions, quantified by the modified combustion efficiency (MCE), we found that aerosol hygroscopicity depends on both fuel types and to some extent on burning conditions. For similar MCE, cow dung has a consistently larger value of hygroscopicity compared to Eucalyptus. Hygroscopicity measurements ranged from 0.024 to 0.577 for MCE measurements that ranged from 0.73 to 0.99. Specifically, sub-saturated hygroscopicity parameter values for cow dung are 0.024–0.131 and Eucalyptus are 0.012–0.300, while supersaturated hygroscopicity parameter values for cow dung are 0.071–0.577 and Eucalyptus are 0.021–0.494. There is a clear increase in hygroscopicity with increasing MCE for supersaturated cow dung measurements using CCNC but the dependence of kappa on MCE is generally inconclusive.

Kinetic Limitations Affect Cloud Condensation Nuclei Activity Measurements Under Low Supersaturation

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

Agricultural Aerosols: The Impact of Farming Activity on Ice Nucleating Particles

Farming activities cause particles such as soil dust and plant material to be emitted into the air. Some of these aerosols can become ice nucleating particles (INPs), serving as seeds for ice and mixed-phase clouds. While there have been ground-based studies of these particles in the western Great Plains and a single air-based study in Indiana, there is a distinct lack of ground-based studies in the Midwest. In Indiana, over two-thirds of the state is farmland, with over 75% of land in Tippecanoe County used for agriculture. Despite farming being such an essential part of life in Indiana, the connection between agricultural activities and INP concentrations in the area has not been explored. Using field observations taken at the Purdue Agronomy Center for Research and Education (ACRE), we hope to study the impact of harvesting on INP concentrations in the midwestern United States. The field experiment took place from May to December 2021 at the ACRE site, but this study focuses on three days during the harvesting period. Data was collected via two instruments: the SPectrometer for Ice Nuclei (SPIN) and the Cloud Condensation Nuclei Counter (CCNC). It appears there is an increase in INP concentrations on days when harvesting occurs, most likely due to an increase in organic and biological particles. It is hoped that the data from this project will provide further insight into the composition and number concentrations of INPs from harvesting through ground-based field observations, as well as insight into INP concentration in the rural Midwest and its climatic impacts.

A single-parameter hygroscopicity model for functionalized insoluble aerosol surfaces

Abstract. The impact of molecular level surface chemistry for aerosol water-uptake and droplet growth is not well understood. In this work, spherical, nonporous, monodisperse polystyrene latex (PSL) particles treated with different surface functional groups are exploited to isolate the effects of aerosol surface chemistry for droplet activation. PSL is effectively water insoluble and changes in the particle surface may be considered a critical factor in the initial water uptake of water-insoluble material. The droplet growth of two surface modified types of PSL (PSL-NH2 and PSL-COOH) along with plain PSL was measured in a supersaturated environment with a Cloud Condensation Nuclei Counter (CCNC). Three droplet growth models – traditional Köhler (TK), Flory–Huggins Köhler (FHK) and the Frenkel–Halsey–Hill adsorption theory (FHH-AT) were compared with experimental data. The experimentally determined single hygroscopicity parameter, κ, was found within the range from 0.002 to 0.04. The traditional Köhler prediction assumes Raoult's law solute dissolution and underestimates the water-uptake ability of the PSL particles. FHK can be applied to polymeric aerosol; however, FHK assumes that the polymer is soluble and hydrophilic. Thus, the FHK model generates a negative result for hydrophobic PSL and predicts non-activation behavior that disagrees with the experimental observation. The FHH-AT model assumes that a particle is water insoluble and can be fit with two empirical parameters (AFHH and BFHH). The FHH-AT prediction agrees with the experimental data and can differentiate the water uptake behavior of the particles owing to surface modification of PSL surface. PSL-NH2 exhibits slightly higher hygroscopicity than the PSL-COOH, whereas plain PSL is the least hygroscopic among the three. This result is consistent with the polarity of surface functional groups and their affinity to water molecules. Thus, changes in AFHH and BFHH can be quantified when surface modification is isolated for the study of water-uptake. The fitted AFHH for PSL-NH2, PSL-COOH, and plain PSL is 0.23, 0.21, and 0.18 when BFHH is unity. To simplify the use of FHH-AT for use in cloud activation models, we also present and test a new single parameter framework for insoluble compounds, κFHH. κFHH is within 5 % agreement of the experimental data and can be applied to describe a single-parameter hygroscopicity for water-insoluble aerosol with surface modified properties.

On the evolution of sub- and super-saturated water uptake of secondary organic aerosol in chamber experiments from mixed precursors

Abstract. To better understand the chemical controls of sub- and super-saturated aerosol water uptake, we designed and conducted a series of chamber experiments to investigate the evolution of secondary organic aerosol (SOA) particle physicochemical properties during photo-oxidation of single and mixed biogenic (α-pinene, isoprene) and anthropogenic (o-cresol) volatile organic compounds (VOCs) in the presence of ammonium sulfate seeds. During the 6 h experiments, the cloud condensation nuclei (CCN) activity at super-saturation of water (0.1 %–0.5 %), hygroscopic growth factor at 90 % relative humidity (RH), and non-refractory PM1 chemical composition were recorded concurrently. Attempts to use the hygroscopicity parameter κ to reconcile water uptake ability below and above water saturation from various VOC precursor systems were made, aiming to predict the CCN activity from the sub-saturated hygroscopicity. The thermodynamic model AIOMFAC (aerosol inorganic-organic mixtures functional groups activity coefficients) was used to simulate κ values of model compound mixtures to compare with the observation and to isolate the controlling factors of water uptake at different RHs. The sub- and super-saturated water uptake (in terms of both κHTDMA and κCCN) were mainly controlled by the SOA mass fraction, which depended on the SOA production rate of the precursors, and the SOA composition played a second-order role. For the reconciliation of κHTDMA and κCCN, the κHTDMA/κCCN ratio increased with the SOA mass fraction and this was observed in all investigated single and mixed VOC systems, independent of initial VOC concentrations and sources. For all VOC systems, the mean κHTDMA of aerosol particles was ∼25 % lower than the κCCN at the beginning of the experiments with inorganic seeds. With the increase of condensed SOA on inorganic seed particles throughout the experiments, the discrepancy of κHTDMA and κCCN became weaker (down to ∼0 %) and finally the mean κHTDMA was ∼60 % higher than κCCN on average when the SOA mass fraction approached ∼0.8. As indicated by AIOMFAC model simulations, non-ideality alone cannot fully explain the κ discrepancy at high SOA mass fraction (0.8). A good agreement in κCCN between model and observation was achieved by doubling the molecular weight of the model compounds or by reducing the dry particle size in the CCN counter. This indicates that the evaporation of semi-volatile organics in the CCN counter together with non-ideality could have led to the observed κ discrepancy. As a result, the predicted CCN number concentrations from the κHTDMA and particle number size distribution were ∼10 % lower than CCN counter measurement on average at the beginning, and further even turned to an overestimation of ∼20 % on average when the SOA mass fraction was ∼0.8. This chemical composition-dependent performances of the κ-Köhler approach on CCN prediction can introduce a variable uncertainty in predicting cloud droplet numbers from the sub-saturated water uptake, the influence of which on models still needs to be investigated.

Hygroscopic growth and CCN activity of secondary organic aerosol produced from dark ozonolysis of γ-terpinene

The hygroscopic growth factor (GF) and cloud condensation nuclei (CCN) activity of secondary organic aerosol (SOA) particles produced during dark ozonolysis of γ-terpinene under different reaction conditions were investigated. The SOA particles were produced in the presence or absence of cyclohexane, an OH scavenger; 1,3,5-trimethylbenzene, an anthropogenic volatile organic compound; and (NH4)2SO4 seed particles. A hygroscopicity tandem differential mobility analyzer was used to determine the GFs of the SOA particles at RHs ≤ 93%. For some experiments, a CCN counter was used for size-resolved measurement of CCN activation at supersaturation (S) in the range of 0.1 to 1%. The single hygroscopicity parameter κ was derived from both the GF and CCN measurements. Under subsaturated conditions, all the SOA (except those in the presence of the (NH4)2SO4 seeds) showed small GF values. These GFs demonstrated that SOA mass loading affected the GF. A decrease in the SOA mass loading led to increased GF and corresponding κGFvalues. However, in a supersaturation regime, the SOA mass loading and the size of the particles did not significantly alter the CCN activity of the SOA. Our CCN measurements showed higher κCCN values (κCCN = 0.20–0.24) than those observed in most monoterpene ozonolysis studies (κCCN = 0.1–0.14). This difference may have been due to the presence of the two endocyclic double bonds in the γ-terpinene structure, which may have affected the SOA chemical composition, in contrast to monoterpenes that contain an exocyclic double bond. Our comparisons of sub- and supersaturated conditions showed a larger range of κ values than other experiments. Average κCCN/κGF ratios of ~7 and 14 were obtained in the unseeded SOA experiments at low and high SOA mass loadings, respectively. The average κCCN of 0.23 indicated that the SOA produced during ozonolysis of γ-terpinene exhibited fairly high CCN activity.

Wetting properties of fresh urban soot particles: Evaluation based on critical supersaturation and observation of surface trace materials

Soot particles strongly absorb solar radiation and contribute to global warming. Also, wetting properties of soot at emission can affect its lifetime. We investigated surface conditions related to wetting and hydrophobic properties of fresh soot using data from measurements taken in Tokyo. A cloud condensation nuclei (CCN) counter was used to clarify surface conditions of particles composed mainly of water-insoluble (WI) materials: total and active particles as CCN around critical supersaturation (Sc) of 203-nm-diameter WI particles. Averaged number fractions of inactivated particles as CCN at 1.05% supersaturation (SS), which is Sc of hydrophilic WI particles, were estimated as 1.4%. Number fractions of inactive particles changed less at 1.78%SS during rush hour and increased at 0.89%SS, implying that most of the WI particles included small amounts of water-soluble (WS) materials rather than being completely hydrophobic. Based on transmission electron microscope (TEM) analysis of samples collected during rush hour, 69% of the mostly bare soot particles had Na or K small domains that are regarded as originating in fossil fuels. Based on water dialysis analysis results, some Na and K on soot were WS. Combination results with CCN measurements suggest that these WS materials decrease the Sc of soot. Moreover, the morphological structure of sulfate covering Na and K domains on the soot surface implicates pre-existing sodium and potassium compounds on soot as a trigger of soot aging. However, inactive particles at Sc at poor-hydrophilic particles and soot particles composed solely of WI materials on TEM samples were also found, although they were minor. Such particles, which are unfavorable for obtaining a wettable surface, might retain non-hygroscopicity for a longer period in the atmosphere. Evaluation of long-range soot transport can benefit from consideration of slight and inhomogeneous differences of chemical compounds on soot that occur along with their emission.

Calibration and evaluation of a broad supersaturation scanning (BS2) cloud condensation nuclei counter for rapid measurement of particle hygroscopicity and cloud condensation nuclei (CCN) activity

Abstract. For understanding and assessing aerosol–cloud interactions and their impact on climate, reliable measurement data on aerosol particle hygroscopicity and cloud condensation nuclei (CCN) activity are required. The CCN activity of aerosol particles can be determined by scanning particle size and supersaturation (S) in CCN measurements. Compared to an existing differential mobility analyzer (DMA) with CCN activity measurement, a broad supersaturation scanning CCN (BS2-CCN) system, in which particles are exposed to a range of S simultaneously, can measure the CCN activity with a high time resolution. Based on a monotonic relation between the activation supersaturation of aerosol particles (Saerosol) and the activated fraction (Fact) of the BS2-CCN measurement, we can derive κ, a single hygroscopicity parameter, directly. Here, we describe how the BS2-CCN system can be effectively calibrated and which factors can affect the calibration curve (Fact−Saerosol). For calibration, size-resolved CCN measurements with ammonium sulfate and sodium chloride particles are performed under three different thermal gradient (dT) conditions (dT=6, 8, and 10 K). We point out key processes that can affect the calibration curve and thereby need to be considered as follows: first, the shape of the calibration curve is primarily influenced by Smax, the maximum S in the activation tube. We need to determine appropriate Smax depending on the particle size and κ to be investigated. To minimize the effect of multiply charged particles, a small geometric mean diameter (Dg) and geometric standard deviation (σg) in number size distribution are recommended when generating the calibration aerosols. Last, Fact is affected by particle number concentration and has a decreasing rate of 0.02 per 100 cm−3 due to the water consumption in the activation tube. For evaluating the BS2-CCN system, intercomparison experiments between typical DMA-CCN and BS2-CCN measurements were performed with a laboratory-generated aerosol mixture and ambient aerosols. Good agreement of κ values between DMA-CCN and BS2-CCN measurements for both experiments shows that the BS2-CCN system can measure CCN activity well compared to the existing measurement method and can measure a broad range of hygroscopicity distributions with a high time resolution (∼1 s vs. a few minutes for a standard CCN activity measurement). As the hygroscopicity can be used as a proxy for the chemical composition, our method can also serve as a complementary approach for fast and size-resolved detection and estimation of aerosol chemical composition.

Investigation of physico-chemical characteristics and associated CCN activation for different combustion sources through Chamber experiment approach

The aerosol physico-chemical properties along with their CCN activation characteristics were studied for different combustion source types such as Diesel Generator (DG), wood, leaf, charcoal, grass and cow dung through chamber-based experiment. Aethalometer (AE-33), High resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS), scanning mobility particle sizer (SMPS) and cloud condensation nuclei (CCN) counter were connected in line to derive the absorption properties, chemical composition, size distribution and CCN number concentrations respectively. Angstrom absorption exponent (AAE) and Angstrom absorption exponent ratio (AAER) were estimated utilizing the Aethalometer data. The analysis reveals that the DG emission was associated with the lowest AAE value (0.92) and the AAE value was highest for cow dung emissions (2.15). AAER, a ratio of AAE at longer wavelengths (660–950 nm) to smaller wavelengths (370-660 nm), showed value < 1 for most of biomass burning types, whereas, the AAER value was >1 for DG emission. The chemical composition data reveals that the organics contribute more than 90% to most of the combustion sources except charcoal, for which the organic contribution was only 78%. High-resolution data analysis reveals that leaf burning was associated with the highest f44 fraction indicating the emitted organic aerosols contain more oxygen. The chemical composition derived hygroscopicity parameter (κ) was estimated to be highest for charcoal emissions and lowest for diesel and cooking emissions. Hygroscopicity parameter (κ) was also evaluated utilizing CCN and SMPS data. The CCN activation and size distribution analysis revealed that the CCN activation of cow dung was highest at 0.1% and 0.3% SS, this is associated with the higher geometric mean diameter (GMD) of emitted aerosols, indicating the importance of size compared to the chemical composition. The activation fraction of charcoal emission was found to be higher than DG emission in these super-saturations, indicating the importance of hygroscopicity in addition to size for governing the CCN activation when the GMD is on the lower side.

CCN and INP activity of middle eastern soil dust

The term mineral dust encompasses a myriad of particle compositions from both fertile and arid regions. Due to this diversity, the quantitative understanding of mineral dust as Cloud Condensation Nuclei (CCN) and Ice Nucleating Particles (INPs) in the Earth’s atmosphere demand further investigation. This study characterizes the CCN and INP activity of mineral dust particles from samples collected from one of the Earth’s major arid regions, Saudi Arabia. Samples were size selected at particle diameters (Dp) of 300, 700, and 950 nm and introduced into a Cloud Condensation Nuclei Counter (CCNC) and a SPectrometer for Ice Nuclei (SPIN) chamber to investigate cloud nucleation activity. The chemical composition of the particles was analyzed with laser mass spectrometry and mineralogical information was provided by polarized light microscopy. Transmission electron microscopy was used to ascertain particle morphology. Each particle size was exposed to water supersaturations of 0.06–1.0% in the CCNC and to ice supersaturation ratios of 1.1 to 1.5 at temperatures from −25 to −42 °C in SPIN. The CCN activity ranged from hygroscopicity values (κ) of 0.001 to 0.01. This is towards the lower range of critical supersaturations found for other mineral dust samples from e.g. the Sahara, North Africa, China and Asia. The INP activity, defined by fractional activation and supersaturation at the onset of ice nucleation was in the range of other natural mineral dusts (e.g., the Sahara, Canary Islands), and somewhat lower than industrially processed Arizona Test Dust. This study highlights the importance of considering size-resolved compositional data when interpreting the cloud-nucleation activity of natural mineral and soil dusts.

The important roles of surface tension and growth rate in the contribution of new particle formation (NPF) to cloud condensation nuclei (CCN) number concentration: evidence from field measurements in southern China

Abstract. The contribution of new particle formation (NPF) to cloud condensation nuclei (CCN) number concentration (NCCN) varies largely under different environments and depends on several key factors such as formation rate (J), growth rate (GR), distribution of preexisting particles, and properties of new particles during NPF events. This study investigates the contribution of NPF to the NCCN and its controlling factors based on measurements conducted at the Heshan supersite, in the Pearl River Delta (PRD) region of China during fall 2019. The size-resolved cloud condensation nuclei activity and size-resolved particle hygroscopicity were measured by a cloud condensation nuclei counter (CCNc) and a hygroscopic tandem differential mobility analyzer (HTDMA), respectively, along with a scanning mobility particle sizer (SMPS) and a diethylene glycol scanning mobility particle sizer (DEG-SMPS) for particle number size distribution (PNSD). A typical NPF event on 29 October was chosen to investigate the contribution of the NPF to NCCN under several supersaturation (SS) ratios. Two particle properties (hygroscopicity and surface tension) affect CCN activation with the latter being more important in terms of the CCN concentration (NCCN). A lower value of surface tension (i.e., 0.06 N m−1) than the pure-water assumption (0.073 N m−1) could increase the NCCN at SS = 1.0 % by about 20 % during the nonevent period and by about 40 % during the event. In addition, an earlier peak time corresponding to a lower critical diameter (D50) was also observed. The results show that high formation rate, growth rate, and low background particle concentration lead to high number concentrations of newly formed particles. The high growth rate was found to have the most significant impact on the NCCN, which can be attributed to the fact that a higher growth rate can grow particles to the CCN size in a shorter time before they are scavenged by preexisting particles. Two other NPF events (an event on 18 October in this campaign and an event on 12 December 2014 in Panyu) were chosen to perform sensitivity tests under different scenarios (growth rate, formation rate, and background particle concentration). The calculated NCCN at SS = 1.0 % on 12 December 2014 was significantly lower than that from the other two events. The event on 12 December was re-simulated using the growth rate taken from the event on 18 October which resulted in similar CCN concentrations between the two events (12 December and 18 October), implying that the growth rate is the major impact factor for CCN activation. Our results highlight the importance of growth rate and surface tension when evaluating the contribution of NPF to the NCCN.

Mathematical derivation and physical interpretation of particle size-resolved activation ratio based on particle hygroscopicity distribution: Application on global characterization of CCN activity

Size-resolved particle activation ratio (SPAR), the size-dependent ability of aerosol particles to form cloud condensation nuclei (CCN), is generally parameterized by a formula with sigmoidal shape with three key parameters. However, our understanding about the intrinsic relationship between the sigmoidal shape function and aerosol hygroscopicity distribution remains incomplete. In this study, the relationship between SPAR and particle hygroscopicity distribution is mathematically derived and relationships between key parameters for SPAR and particle hygroscopicity distribution are manifested, making it clear for the physical understanding of key CCN spectral characteristics. On the basis of the mathematically derived SPAR parameterization, a simplified method to calculate SPAR parameters (including maximum activation fraction (MAF), critical diameter and its heterogeneity of CCN-active particles) based on hygroscopicity distribution data is proposed. This simplified method is applied to Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) field measurement datasets around the world for the meta-analysis of regional and seasonal characteristics of CCN activity. It was found that, for CCN-active particles in polluted regions, the MAF can reach lower values, and the variations of both hygroscopicity and its heterogeneity can be larger, compared with those in clean regions. In summer, the MAF and the hygroscopicity of CCN can reach higher values than those in winter. In addition, the variations of SPAR parameters among different campaigns are large and thus measurements of CCN Counter or HTDMA are needed to specify the SPAR parameters at a specific site during a specific period. The bulk CCN activity at different SSs are also calculated based on the calculated SPAR by considering the measured particle number size distribution. The mathematical derivation and physical interpretation of SPAR parameterization in this study can further the understanding of CCN activity based on particle hygroscopicity distribution. The proposed simplified method to calculate SPAR parameters based on HTDMA measurements allows meta-analysis of SPAR parameters and helps expand the CCN activity datasets around the world.

First surface measurement of variation of Cloud Condensation Nuclei (CCN) concentration over the Pristine Himalayan region of Garhwal, Uttarakhand, India

A Droplet Measurement Technology (DMT) Cloud Condensation Nuclei Counter (CCNC) was deployed to measure cloud condensation nuclei (CCN) for the first time in the pristine Himalayan region at Himalayan Clouds Observatory (HCO), Swami Ram Tirtha (SRT) Campus (30°34′ N, 78°41′ E, 1706 m AMSL), Hemvati Nandan Bahuguna (HNB) Garhwal University, Badshahithaul, Tehri Garhwal, Uttarakhand, India. The CCN concentration (NCCN) was observed at four supersaturation levels (SS: 0.2, 0.5, 0.8, and 1.0%). In this study, we reported CCN concentration at 0.5% SS in different weather conditions from Aug 01, 2018 to Jun 30, 2019. During this observation period, the monthly averaged value of CCN concentration ranged between 1098.3 ± 448.9 cm−3 (mean ± SD) and 3842.9 ± 2512.9 cm−3. It covers a significantly wide range of daily averaged concentrations from the minimum concentration of 43.84 cm−3 (during heavy wet scavenging due to snowfall) to maximum concentration of 17000 cm−3 (during the events of a forest fire) at the observation site. The highest CCN concentration is observed at the time of sunrise (~07:00 a.m.) and after the sunset (~07:00 p.m.) for the diurnal variation of monsoon, post-monsoon, and winter season. Pre-monsoon season shows peak values at 10:00 a.m. and at 07:00 p.m. with higher concentrations at night hours. The possible reasons for maximum concentration in morning and evening time could be upliftment and settlement of CCN because of the convection process, anthropogenic emission, vehicular emission, and biomass burning in the residential area and valley region adjacent to HCO, Badshahithaul. The highest CCN concentration (3842.9 ± 2513 cm−3) values of the whole observation period were observed in May 2019. It was significantly affected by the heavy fire activities over the Uttarakhand and nearby IGP regions. Diurnal variation of CCN concentration during the HFAD shows higher values in the night time differing from the diurnal pattern of CCN for other months of the observation period. The long-range transport of air mass could also contribute to the high CCN concentration values, as found through the five-day air mass backward trajectory analysis. The lowest value of CCN concentration corresponds to the heavy rains and snowfall days, possibly caused by extensive wet scavenging. Cluster analysis of the air mass trajectories used for the allocation and classification of the possible sources of pollutants reaching the observation site. The highest fraction of CCN concentration (more than 2000 cm−3) corresponds to the air mass from the arid and semi-arid regions of Asian countries. Large air mass fraction (~40–60%) with moderate CCN concentration was received from northwestern IGP region and foothills of central Himalaya.