scholarly journals Aerosol hygroscopicity and CCN activity obtained from a combination analysis based on size-resolved CCN and aerosol chemical composition observations during the AC<sup>3</sup>Exp13 campaign

2014 ◽  
Vol 14 (10) ◽  
pp. 14889-14931 ◽  
Author(s):  
F. Zhang ◽  
Z. Li ◽  
R. J. Li ◽  
L. Sun ◽  
C. Zhao ◽  
...  

Abstract. Aerosol hygroscopicity and cloud condensation nuclei (CCN) activity under clean conditions and polluted events are investigated based on size-resolved CCN and aerosol chemical composition observations during the Aerosol-CCN-Cloud Closure Experiment (AC3Exp) campaign conducted at Xianghe, China in summer 2013. About 14–22% of aerosol particles during the campaign are of externally mixed CCN-inactive particles that cannot serve as CCN under atmospheric typical supersaturation (SS) of ∼0.4%. A high sensitivity of Maximum activation fractions (MAF) to SS under polluted conditions has been observed. The pollutants can cause a maximum MAF decrease of 25–30% (at SS = 0.08%). Hygroscopicity parameter kappa (κ) are about 16–35% lower under polluted conditions than under clean conditions for particles in accumulation size range (80–180 nm); however, for particles in nucleation or Aitken size range (30–60 nm), κ is slightly higher under polluted conditions. A non-parallel observation (NPO) CCN closure study shows low correlation coefficient between estimated and observed CCN number concentrations (NCCN). About 30–40% uncertainties in NCCN prediction are associated with the changes of particle composition. A case study shows that CCN activation ratio (AR) increased with the increase of condensation nuclei (CN) number concentrations (NCN) in relatively clean days. In the case, AR exhibited good correlation with κchem, which is calculated from chemical volume fractions, due to particles mainly composed of soluble inorganics. On the contrary, AR declined with increase of NCN during polluted events when particles composed mostly of organics. Meanwhile, AR is closely related to f44, which is the fraction of total organic mass signal at m/z 44 and closely associated with particle organic oxidation level. Our study highlights the importance of aerosols chemical composition on determining the activation properties of aerosol particles, underlining the importance of long-term observation of CCN under different atmospheric environments, especially those with heavy pollution and high CN number concentrations.

2021 ◽  
Vol 21 (14) ◽  
pp. 11289-11302
Author(s):  
Imre Salma ◽  
Wanda Thén ◽  
Máté Vörösmarty ◽  
András Zénó Gyöngyösi

Abstract. Collocated measurements using a condensation particle counter, differential mobility particle sizer and cloud condensation nuclei counter were realised in parallel in central Budapest from 15 April 2019 to 14 April 2020 to gain insight into the cloud activation properties of urban aerosol particles. The median total particle number concentration was 10.1 × 103 cm−3. The median concentrations of cloud condensation nuclei (CCN) at water vapour supersaturation (S) values of 0.1 %, 0.2 %, 0.3 %, 0.5 % and 1.0 % were 0.59, 1.09, 1.39, 1.80 and 2.5 × 103 cm−3, respectively. The CCN concentrations represented 7–27 % of all particles. The CCN concentrations were considerably larger but the activation fractions were systematically substantially smaller than observed in regional or remote locations. The effective critical dry particle diameters (dc,eff) were derived utilising the CCN concentrations and particle number size distributions. Their median values at the five supersaturation values considered were 207, 149, 126, 105 and 80 nm, respectively; all of these diameters were positioned within the accumulation mode of the typical particle number size distribution. Their frequency distributions revealed a single peak for which the geometric standard deviation increased monotonically with S. This broadening indicated high time variability in the activating properties of smaller particles. The frequency distributions also showed fine structure, with several compositional elements that seemed to reveal a consistent or monotonical tendency with S. The relationships between the critical S and dc,eff suggest that urban aerosol particles in Budapest with diameters larger than approximately 130 nm showed similar hydroscopicity to corresponding continental aerosol particles, whereas smaller particles in Budapest were less hygroscopic than corresponding continental aerosol particles. Only modest seasonal cycling in CCN concentrations and activation fractions was seen, and only for large S values. This cycling likely reflects changes in the number concentration, chemical composition and mixing state of the particles. The seasonal dependencies of dc,eff were featureless, indicating that the droplet activation properties of the urban particles remained more or less the same throughout the year. This is again different from what is seen in non-urban locations. Hygroscopicity parameters (κ values) were computed without determining the time-dependent chemical composition of the particles. The median values for κ were 0.15, 0.10, 0.07, 0.04 and 0.02, respectively, at the five supersaturation values considered. The averages suggested that the larger particles were considerably more hygroscopic than the smaller particles. We found that the κ values for the urban aerosol were substantially smaller than those previously reported for aerosols in regional or remote locations. All of these characteristics can be linked to the specific source composition of particles in cities. The relatively large variability in the hygroscopicity parameters for a given S emphasises that the individual values represent the CCN population in ambient air while the average hygroscopicity parameter mainly corresponds to particles with sizes close to the effective critical dry particle diameter.


2020 ◽  
Vol 20 (10) ◽  
pp. 5911-5922 ◽  
Author(s):  
Hing Cho Cheung ◽  
Charles Chung-Kuang Chou ◽  
Celine Siu Lan Lee ◽  
Wei-Chen Kuo ◽  
Shuenn-Chin Chang

Abstract. The chemical composition of fine particulate matter (PM2.5), the size distribution and number concentration of aerosol particles (NCN), and the number concentration of cloud condensation nuclei (NCCN) were measured at the northern tip of Taiwan during an intensive observation experiment from April 2017 to March 2018. The parameters of aerosol hygroscopicity (i.e., activation ratio, activation diameter and kappa of CCN) were retrieved from the measurements. Significant variations were found in the hygroscopicity of aerosols (kappa – κ – of 0.18–0.56, for water vapor supersaturation – SS – of 0.12 %–0.80 %), which were subject to various pollution sources, including aged air pollutants originating in eastern and northern China and transported by the Asian continental outflows and fresh particles emitted from local sources and distributed by land–sea breeze circulations as well as produced by processes of new particle formation (NPF). Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aerosols associated with Asian continental outflows were characterized by lower NCN and NCCN values and by higher kappa values of CCN, whereas higher NCN and NCCN values with lower kappa values of CCN were observed in the aerosols associated with local air masses. Besides, it was revealed that the kappa value of CCN exhibited a decrease during the early stage of an event of new particle formation, which turned to an increasing trend over the later period. The distinct features in the hygroscopicity of aerosols were found to be consistent with the characteristics in the chemical composition of PM2.5. This study has depicted a clear seasonal characteristic of hygroscopicity and CCN activity under the influence of a complex mixture of pollutants from different regional and/or local pollution sources. Nevertheless, the mixing state and chemical composition of the aerosols critically influence the aerosol hygroscopicity, and further investigations are necessary to elucidate the atmospheric processing involved in the CCN activation in coastal areas.


2019 ◽  
Vol 19 (24) ◽  
pp. 15545-15567 ◽  
Author(s):  
Franz Friebel ◽  
Prem Lobo ◽  
David Neubauer ◽  
Ulrike Lohmann ◽  
Saskia Drossaart van Dusseldorp ◽  
...  

Abstract. The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted into the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of 1 week, requiring tailored experiments that cover this time span. This work presents results on the ability of two types of soot, obtained using a miniCAST soot generator, to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone (O3) and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size selection of particles prior to the aging step. Particles of 100 nm diameter and rich in organic carbon (OC) that were initially CCN inactive showed significant CCN activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of O3. While this process was not affected by different levels of relative humidity in the range of 5 %–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC content required an approximately 4-fold longer aging duration to show CCN activity at the same SS. Prior to the slow change in the CCN activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (<3 m3). Implementation of our measurement results in a global aerosol-climate model, ECHAM6.3-HAM2.3, showed a statistically significant increase in the regional and global CCN burden and cloud droplet number concentration.


2019 ◽  
Author(s):  
Franz Friebel ◽  
Prem Lobo ◽  
David Neubauer ◽  
Ulrike Lohmann ◽  
Saskia Drossaart van Dusseldorp ◽  
...  

Abstract. The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted to the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of one week, demanding tailored experiments that cover this time span. This work presents results on the ability of two types of soot to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size-selection of particles prior to the aging step. 100 nm particles rich in organic carbon (OC) that were initially CCN-inactive showed significant CCN-activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of ozone. While this process was not affected by different levels of relative humidity in the range 5–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC-content demanded an approximately four-fold longer aging duration to show CCN-activity for the same SS. Prior to the slow change in the CCN-activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR-approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (


2013 ◽  
Vol 13 (9) ◽  
pp. 23817-23843 ◽  
Author(s):  
E. J. T. Levin ◽  
A. J. Prenni ◽  
B. Palm ◽  
D. Day ◽  
P. Campuzano-Jost ◽  
...  

Abstract. Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions of non-refractory components were between 70–90%. Corresponding aerosol hygroscopicity was observed to range from κ = 0.15–0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an Aerosol Mass Spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study with an assumed value of κorg = 0.13 resulting in the best agreement.


2021 ◽  
Author(s):  
Najin Kim ◽  
Yafang Cheng ◽  
Nan Ma ◽  
Mira L. Pöhlker ◽  
Thomas Klimach ◽  
...  

Abstract. For understanding and assessing aerosol-cloud interactions and their impact on climate, reliable measurement data of 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 the existing differential mobility analyzer (DMA)-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 the 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 particle size and κ to be investigated. To minimize the effect of multiply charged particles, small geometric mean diameter (𝐷𝑔) and 𝜎𝑔 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 0.02/100 cm−3 due to the water consumption in the activation tube. For evaluating the BS2-CCN system, inter-comparison experiments between typical DMA-CCN and BS2-CCN measurement were performed with the laboratory-generated aerosol mixture and ambient aerosols. Good agreements of κ values between DMA-CCN and BS2-CCN measurements for both experiments show that the BS2-CCN system can measure CCN activity well compared to the existing measurement, and can measure a broad range of hygroscopicity distribution with a high time-resolution (~1 second vs. 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/estimation of aerosol chemical composition.


2011 ◽  
Vol 11 (21) ◽  
pp. 11023-11039 ◽  
Author(s):  
S. S. Gunthe ◽  
D. Rose ◽  
H. Su ◽  
R. M. Garland ◽  
P. Achtert ◽  
...  

Abstract. Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. CCN properties were measured and characterized during the CAREBeijing-2006 campaign at a regional site south of the megacity of Beijing, China. Size-resolved CCN efficiency spectra recorded for a supersaturation range of S=0.07% to 0.86% yielded average activation diameters in the range of 190 nm to 45 nm. The corresponding effective hygroscopicity parameters (κ) exhibited a strong size dependence ranging from ~0.25 in the Aitken size range to ~0.45 in the accumulation size range. The campaign average value (κ =0.3 ± 0.1) was similar to the values observed and modeled for other populated continental regions. The hygroscopicity parameters derived from the CCN measurements were consistent with chemical composition data recorded by an aerosol mass spectrometer (AMS) and thermo-optical measurements of apparent elemental and organic carbon (EC and OC). The CCN hygroscopicity and its size dependence could be parameterized as a function of only AMS based organic and inorganic mass fractions (forg, finorg) using the simple mixing rule κp ≈ 0.1 · forg + 0.7 · finorg. When the measured air masses originated from the north and passed rapidly over the center of Beijing (fresh city pollution), the average particle hygroscopicity was reduced (κ = 0.2 ± 0.1), which is consistent with enhanced mass fractions of organic compounds (~50%) and EC (~30%) in the fine particulate matter (PM1). Moreover, substantial fractions of externally mixed weakly CCN-active particles were observed at low supersaturation (S=0.07%), which can be explained by the presence of freshly emitted soot particles with very low hygroscopicity (κ < 0.1). Particles in stagnant air from the industrialized region south of Beijing (aged regional pollution) were on average larger and more hygroscopic, which is consistent with enhanced mass fractions (~60%) of soluble inorganic ions (mostly sulfate, ammonium, and nitrate). Accordingly, the number concentration of CCN in aged air from the megacity region was higher than in fresh city outflow ((2.5–9.9) × 103 cm−3 vs. (0.4–8.3) × 103 cm−3 for S=0.07–0.86%) although the total aerosol particle number concentration was lower (1.2 × 104 cm−3 vs. 2.3 × 104 cm−3). A comparison with related studies suggests that the fresh outflow from Chinese urban centers generally may contain more, but smaller and less hygroscopic aerosol particles and thus fewer CCN than the aged outflow from megacity regions.


2018 ◽  
Vol 18 (22) ◽  
pp. 16419-16437 ◽  
Author(s):  
Mingfu Cai ◽  
Haobo Tan ◽  
Chak K. Chan ◽  
Yiming Qin ◽  
Hanbing Xu ◽  
...  

Abstract. A hygroscopic tandem differential mobility analyzer (HTDMA), a scanning mobility cloud condensation nuclei (CCN) analyzer (SMCA), and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were used to, respectively, measure the hygroscopicity, condensation nuclei activation, and chemical composition of aerosol particles at the Panyu site in the Pearl River Delta region during wintertime 2014. The distribution of the size-resolved CCN at four supersaturations (SSs of 0.1 %, 0.2 %, 0.4 %, and 0.7 %) and the aerosol particle size distribution were obtained by the SMCA. The hygroscopicity parameter κ (κCCN, κHTDMA, and κAMS) was, respectively, calculated based upon the SMCA, HTDMA, and AMS measurements. The results showed that the κHTDMA value was slightly smaller than the κCCN one at all diameters and for particles larger than 100 nm, and the κAMS value was significantly smaller than the others (κCCN and κHTDMA), which could be attributed to the underestimated hygroscopicity of the organics (κorg). The activation ratio (AR) calculated from the growth factor – probability density function (Gf-PDF) without surface tension correction was found to be lower than that from the CCN measurements, due most likely to the uncorrected surface tension (σs∕a) that did not consider the surfactant effects of the organic compounds. We demonstrated that better agreement between the calculated and measured ARs could be obtained by adjusting σs∕a. Various schemes were proposed to predict the CCN number concentration (NCCN) based on the HTDMA and AMS measurements. In general, the predicted NCCN agreed reasonably well with the corresponding measured ones using different schemes. For the HTDMA measurements, the NCCN value predicted from the real-time AR measurements was slightly smaller (∼6.8 %) than that from the activation diameter (D50) method due to the assumed internal mixing in the D50 prediction. The NCCN values predicted from bulk chemical composition of PM1 were higher (∼11.5 %) than those from size-resolved composition measured by the AMS because a significant fraction of PM1 was composed of inorganic matter. The NCCN values calculated from AMS measurement were underpredicted at 0.1 % and 0.2 % supersaturations, which could be due to underestimation of κorg and overestimation of σs∕a. For SS values of 0.4 % and 0.7 %, slight overpredicted NCCN values were found because of the internal mixing assumption. Our results highlight the need for accurately evaluating the effects of organics on both the hygroscopic parameter κ and the surface tension σ in order to accurately predict CCN activity.


2019 ◽  
Author(s):  
Xianda Gong ◽  
Heike Wex ◽  
Thomas Müller ◽  
Alfred Wiedensohler ◽  
Kristina Höhler ◽  
...  

Abstract. As part of the A-LIFE (Absorbing aerosol layers in a changing climate: aging, lifetime and dynamics) campaign, ground-based measurements were carried out in Paphos, Cyprus, for characterizing the abundance, properties and sources of aerosol particles in general, and cloud condensation nuclei (CCN) and ice nucleating particles (INP), in particular. New particle formation (NPF) events with subsequent growth of the particles into the CCN size range were observed. Aitken mode particles featured κ values of 0.21 to 0.29, indicating the presence of organic materials. Accumulation mode particles featured a higher hygroscopicity parameter, with a median κ value of 0.57, suggesting the presence of sulfate. A clear downward trend of κ with increasing supersaturation and decreasing dcrit was found. Super-micron particles originated mainly from sea spray aerosol (SSA) and partly from mineral dust. INP concentrations (NINP) were measured in the temperature range from −6.5 to −26.5 ℃, using two freezing array type instruments. NINP at a particular temperature span around 1 order of magnitude below −20 ℃, and about 2 orders of magnitude at warmer temperatures (T > −18 ℃). Few samples showed elevated concentrations at temperatures > −15 ℃, which suggests a significant contribution of biological particles to the INP population, which possibly could originate from Cyprus. Both measured temperature spectra and NINP probability density functions (PDFs) indicate that the observed INP (ice active in the temperature range between −15 and −20 ℃) mainly originate from long-range transport. There was no correlation between NINP and particle number concentration in the size range > 500 nm (N> 500 nm). Parameterizations based on N> 500 nm were found to overestimate NINP by about 1 to 2 orders of magnitude. There was also no correlation between NINP and particle surface area concentration. The ice active surface site density (ns) for the anthropogenically polluted aerosol encountered in this study is about 1 to 3 orders of magnitude lower than the ns found for dust aerosol particles in previous studies. This suggests that observed NINP-PDFs as those derived here could be a better choice for modelling NINP if the aerosol particle composition is unknown or uncertain.


2014 ◽  
Vol 14 (5) ◽  
pp. 2657-2667 ◽  
Author(s):  
E. J. T. Levin ◽  
A. J. Prenni ◽  
B. B. Palm ◽  
D. A. Day ◽  
P. Campuzano-Jost ◽  
...  

Abstract. Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen–Rocky Mountain Biogenic Aerosol Study) campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions were between 70 and 90%. Corresponding aerosol hygroscopicity was observed to be in the range κ = 0.15–0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an aerosol mass spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study, with an assumed value of κorg = 0.13 resulting in the best agreement.


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