Condensation Nucleus Counter Research Articles

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.

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.

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.

Measurement report: An exploratory study of fluorescence and cloud condensation nuclei activity of urban aerosols in San Juan, Puerto Rico

Abstract. Many atmospheric aerosols are cloud condensation nuclei (CCN), capable of activating as cloud droplets when the relative humidity exceeds 100 %. Some primary biological aerosol particles (PBAPs), such as plant spores, pollen, or bacteria, have been identified as such CCN. Urban environments are a source of these bioaerosols, some of which are naturally produced by the local flora or are transported from surrounding regions and others of which are a result of human activities. In the latter case, open sewage, uncovered garbage, mold or other products of such activities can be a source of PBAPs. There have been relatively few studies, especially in the tropics, where PBAPs and CCN have been simultaneously studied to establish a causal link between the two. The metropolis of San Juan, Puerto Rico, is one such urban area with a population of 2 448 000 people (as of 2020). To better understand the fluorescent characteristics and cloud-forming efficiency of aerosols in this region, measurements with a wideband integrated bioaerosol spectrometer (WIBS), a condensation nuclei (CN) counter and a CCN spectrometer were made at the University of Puerto Rico – Río Piedras Campus. Results show that the CCN / CN activation ratio and the fraction of fluorescing aerosol particles (FAPs) have repetitive daily trends when the FAP fraction is positively correlated with relative humidity and negatively correlated with wind speed, consistent with previous studies of fungi spores collected on substrates. The results from this pilot study highlight the capabilities of ultraviolet-induced fluorescence (UV-IF) measurements for characterizing the properties of FAPs as they relate to the daily evolution of PBAPs. The use of multiple excitation and emission wavelengths, along with shape detection, allows the differentiation of different PBAP types. These measurements, evaluated with respect to previous, substrate-based analysis of the local fungal and pollen spores, have established a preliminary database of measurements that future, longer-term studies will build upon.

Quantitative Fit Test of a 3D Printed Frame Fitted Over a Surgical Mask: An Alternative Option to N95 Respirator.

Background COVID-19 has spread worldwide and caused severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) led to numerous dead cases. However, with the new COVID-19 outbreaks, there is a shortage of personal protective equipment (PPE) especially N95 masks worldwide including Thailand. This issue had placed the health professional in great need of an alternative mask. Aim This study aimed to measure the fit factor of 3D printed frames by quantitative fit testing (QNFT) to find an alternative facemask by using a mask fitter together with 2 different kinds of the American Society for Testing and Materials (ASTM) level 1 surgical mask. Materials and Methods Two commonly used surgical masks (Sultan Com-Fit Super Sensitive Ear Loop Mask or “White Mask Group,” not water-resistant, and Sultan Blue Com-Fit Super High Filtration Ear Loop Mask or “Blue Mask Group,” water-resistant) with and without 3D printed frame covering. The fit performance was measured by a quantitative fit test (QNFT) device (PortaCount, model 8048, TSI Incorporated, Minnesota, USA) accepted by the Occupational Safety and Health Administration (OSHA). The PortaCount device, which is based on a miniature continuous flow condensation nucleus counter (CNC), assesses the respiratory fit by comparing the concentration of ambient dust particles outside the surgical mask to the concentration that has leaked into the surgical mask. The ratio of these two concentrations (Cout/Cin) is called the fit factor. A fit factor of a 3D printed frame of at least 100 is required and considered as a pass level. Results We found that the mask fitter improves the overall performance of surgical masks significantly. The improved performance is comparable to that of N95. Conclusion The mask fitter improves the performance of surgical masks. The authors suggested that further study on frame material, shape, and expanded sample size would be beneficial to society.

Activation of sub-3 nm organic particles in the particle size magnifier using humid and dry conditions

The accurate measurement of aerosol particles and clusters smaller than 3 nm in diameter is crucial for the understanding of new particle formation processes. The particle counters used for measuring these particles are typically calibrated with metal or salt particles under dry conditions, which does not always represent the field conditions where these instruments are later used. In this study, we calibrated the A11 nano Condensation Nucleus Counter (nCNC), consisting of the PSM (Particle Size Magnifier) and a laminar flow butanol based CPC (Condensational Particle Counter), with well-defined biogenic oxidation products from β-caryophyllene oxidation and compared it to a calibration with tungsten oxide under the same conditions. The organic particles were detected less efficiently than the inorganic ones. This resulted in a higher cut-off size for β-caryophyllene oxidation products than for tungsten oxide. At the same PSM settings, the cut-off size for tungsten oxide was 1.2 nm and for β-caryophyllene oxidation products 1.9 nm. However, repeating the calibration of the biogenic particles at 13% relative humidity at 31°C, increased their detection efficiency in the PSM, increasing the cut-off diameter to 1.6 nm.Additionally, we present a comparison of the ion concentrations measured with the PSM and the NAIS (Neutral Cluster and Air Ion Spectrometer) during new particle formation experiments in the CLOUD (Cosmics Leaving Outdoors Droplets) chamber. In these experiments, we produced particles from different organic precursors, such as α-pinene, β-caryophyllene and isoprene, as well as iodine. This way, we could determine the shift in cut-off diameter of the PSM for several different atmospherically relevant chemical compounds and compare it to the laboratory calibrations. We saw a diameter shift for the organic precursors of +0.3 nm in the PSM compared to the NAIS. These two approaches agreed well with each other and show that it is important to know the chemical composition of the measured particles to determine the exact size distribution using a supersaturation scanning method.

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.

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.

Distribution Characteristics of Aerosol Size and CCN during the Summer on Mt. Tian and Their Influencing Factors

The aerosol size distribution and cloud condensation nuclei (CCN) number concentration were measured using a wide-range particle spectrometer (WPS) and a cloud condensation nuclei counter (CCNC) on Mt. Tian from 31 July to 9 September, 2019. Combined with meteorological data, distribution characteristics of aerosol size and CCN and their influencing factors were analyzed. The results indicated that the mean aerosol number concentration was 5475.6 ± 5636.5 cm−3. The mean CCN concentrations were 183.7 ± 114.5 cm−3, 729.8 ± 376.1 cm−3, 1630.5 ± 980.5 cm−3, 2162.5 ± 1345.3 cm−3, and 2575.7 ± 1632.9 cm−3 at supersaturation levels of 0.1%, 0.2%, 0.4%, 0.6%, and 0.8%, respectively. The aerosol number size distribution is unimodal, and the dominant particle size is 30–60 nm. Affected by the height of the boundary layer and the valley wind, the diurnal variation in aerosol number concentration shows a unimodal distribution with a peak at 17:00, and the CCN number concentration showed a bimodal distribution with peaks at 18:00 and 21:00. The particle size distribution and supersaturation have a major impact on the activation of the aerosol into CCN. At 0.1% supersaturation (S), the 300–500 nm particles are most likely to activate to CCN. Particles of 100–300 nm are most easily activated at 0.2% (S), while particles of 60–80 nm are most likely activated at high supersaturation (≥0.4%). The concentrations of aerosol and CCN are higher in the northerly wind. Ambient relative humidity (RH) has little relationship with the aerosol activation under high supersaturation. According to N = CSk fitting the CCN spectrum, C = 3297 and k = 0.90 on Mt. Tian, characteristic of the clean continental type.

Application of an O-ring pinch device as a constant-pressure inlet (CPI) for airborne sampling

Abstract. We present a novel and compact design of a constant-pressure inlet (CPI) developed for use in airborne aerosol mass spectrometry. In particular, the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, in which efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hectopascals. The CPI device can also be used in condensation particle counters (CPCs), cloud condensation nucleus counters (CCNCs), and gas-phase sampling instruments across a wide range of altitudes and inlet pressures. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that acts as a critical orifice. The CPI control keeps air pressure and thereby mass flow rate (≈0.1 L min−1) upstream of an aerodynamic lens constant, deviating at most by only ±2 % from a preset value. In our setup, a pressure sensor downstream of the O-ring maintains control of the pinch mechanism via a feedback loop and setpoint conditions are reached within seconds. The device was implemented in a few instruments, which were successfully operated on different research aircraft covering a wide range of ambient pressures, from sea level up to about 55 hPa. Details of operation and the quality of aerosol particle transmission were evaluated by laboratory experiments and in-flight data with a single-particle mass spectrometer.

Influence of the dry aerosol particle size distribution and morphology on the cloud condensation nuclei activation. An experimental and theoretical investigation

Abstract. 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.

An improved parameterization scheme for size-resolved particle activation ratio and its application on comparison study of particle hygroscopicity measurements between HTDMA and DMA-CCNC

Size-resolved Particle Activation Ratio (SPAR), defined as the size-dependence of CCN activity of aerosol particles, is generally parameterized by a scheme that neglects the contribution of nearly-hydrophobic particles. In this paper, it was found that nearly-hydrophobic particles can contribute up to 20% to the CCN activity for large particles and the estimation of particle hygroscopicity would be significantly biased using the original parameterization scheme. An improved parameterization scheme considering the contribution of nearly-hydrophobic particles was proposed and applied on measurements conducted at a rural site in the North China Plain during summer 2013. For hygroscopic particles in range of 50–70 nm diameter, which might be dominated by organic compounds, their number fraction (fn) and midpoint activation diameter (Da) fitted with the improved scheme were up to 20% lower than the parameters fitted with the original scheme. Both parameterization schemes of SPAR were further applied in a comparison study of aerosol hygroscopicity measurements between Cloud Condensation Nuclei (CCN) Counter coupled with Differential Mobility Analyzer (DMA-CCNC) and Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) during the Xianghe Campaign. Applying the improved scheme, the correlations of derived fn for hygroscopic particles between measurements of DMA-CCNC and HTDMA were improved (R increased by up to 0.2 with the uncertainty of the regression to be about 10%). In addition, for particles smaller than 100 nm, the size-dependence of hygroscopicity parameter and the diurnal cycle of fn derived using the improved scheme, based on the DMA-CCNC measurements were more consistent with those derived with the HTDMA measurements. These results highlight the importance of considering nearly-hydrophobic particles in SPAR curves fitting and in the calculation of aerosol hygroscopicity based on DMA-CCNC measurements.