scholarly journals Effects of chemical composition and mixing state on size‐resolved hygroscopicity and cloud condensation nuclei activity of submicron aerosols at a suburban site in northern Japan in summer

2017 ◽  
Vol 122 (17) ◽  
pp. 9301-9318 ◽  
Author(s):  
Astrid Müller ◽  
Yuzo Miyazaki ◽  
Shankar G. Aggarwal ◽  
Yasuyuki Kitamori ◽  
Suresh K. R. Boreddy ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Cloud Condensation Nuclei ◽  
Condensation Nuclei ◽  
Mixing State ◽  
Suburban Site ◽  
Northern Japan

scholarly journals The impact of aerosol size-dependent hygroscopicity and mixing state on the cloud condensation nuclei potential over the Northeast Atlantic

2021 ◽  
Author(s):  
Wei Xu ◽  
Kirsten N. Fossum ◽  
Jurgita Ovadnevaite ◽  
Chunshui Lin ◽  
Ru-Jin Huang ◽  
...  
Keyword(s):  
Biological Activity ◽  
Chemical Composition ◽  
Growth Factor ◽  
Cloud Condensation Nuclei ◽  
Condensation Nuclei ◽  
Mixing State ◽  
Northeast Atlantic ◽  
Size Dependent ◽  
Internal Mixing ◽  
The Impact

Abstract. We present an aerosol cloud condensation nuclei (CCN) closure study over the Northeast Atlantic Ocean using six approximating methods. The CCN number concentrations (NCCN) were measured at four discrete super-saturations (SS, 0.25, 0.5, 0.75 and 1.0 %). Concurrently, aerosol number size distribution, sub-saturation hygroscopic growth factor and bulk PM1 chemical composition were obtained at matching time resolution and after a careful data validation exercise. Method A used a constant bulk hygroscopicity parameter κ of 0.3; method B used bulk PM1 chemical composition measured by an aerosol mass spectrometer (AMS); method C and D utilized a single size (165 nm) growth factor (GF) measured by humidified tandem differential mobility analyzer (HTDMA); method C utilized size-dependent GFs measured at 35, 50, 75, 110 and 165 nm; method E divided the aerosol population into three hygroscopicity modes (near-hydrophobic, more-hygroscopic and sea-salt modes) and the total CCN number in each mode was cumulatively added up; method F used the full size scale GF probability density function (GF-PDF) in the most complex approach. The studied periods included high biological activity and low biological activity seasons in clean marine and polluted continental air masses to represent and discuss the most contrasting aerosol populations. Overall, a good agreement was found between estimated and measured NCCN with a linear regression slopes ranging from 0.64 and 1.6. The temporal variability was captured very well with Pearson's R value ranging from 0.76 to 0.98 depending on the method and air mass type. We further compared the results of using different methods to quantify the impact of size-dependent hygroscopicity and mixing state and found that ignoring size-dependent hygroscopicity induced overestimation of NCCN by up to 12 %, and ignoring a mixing state induced overestimation of NCCN by up to 15 %. The error induced by assuming an internal mixing in highly polluted cases was largely eliminated by dividing the full GF-PDf into three conventional hygroscopic modes while assuming an internal mixing in clean marine aerosol did not induced significant error.

scholarly journals Measured and modelled cloud condensation nuclei number concentration at the high alpine site Jungfraujoch

2010 ◽  
Vol 10 (16) ◽  
pp. 7891-7906 ◽  
Author(s):  
Z. Jurányi ◽  
M. Gysel ◽  
E. Weingartner ◽  
P. F. DeCarlo ◽  
L. Kammermann ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Hydrological Cycle ◽  
Cloud Condensation Nuclei ◽  
Sensitivity Study ◽  
Research Station ◽  
Condensation Nuclei ◽  
Composition Data ◽  
Particle Mobility ◽  
Kohler Theory ◽  
Highly Correlated

Abstract. Atmospheric aerosol particles are able to act as cloud condensation nuclei (CCN) and are therefore important for the climate and the hydrological cycle, but their properties are not fully understood. Total CCN number concentrations at 10 different supersaturations in the range of SS=0.12–1.18% were measured in May 2008 at the remote high alpine research station, Jungfraujoch, Switzerland (3580 m a.s.l.). In this paper, we present a closure study between measured and predicted CCN number concentrations. CCN predictions were done using dry number size distribution (scanning particle mobility sizer, SMPS) and bulk chemical composition data (aerosol mass spectrometer, AMS, and multi-angle absorption photometer, MAAP) in a simplified Köhler theory. The predicted and the measured CCN number concentrations agree very well and are highly correlated. A sensitivity study showed that the temporal variability of the chemical composition at the Jungfraujoch can be neglected for a reliable CCN prediction, whereas it is important to know the mean chemical composition. The exact bias introduced by using a too low or too high hygroscopicity parameter for CCN prediction was further quantified and shown to be substantial for the lowest supersaturation. Despite the high average organic mass fraction (~45%) in the fine mode, there was no indication that the surface tension was substantially reduced at the point of CCN activation. A comparison between hygroscopicity tandem differential mobility analyzer (HTDMA), AMS/MAAP, and CCN derived κ values showed that HTDMA measurements can be used to determine particle hygroscopicity required for CCN predictions if no suitable chemical composition data are available.

scholarly journals Cloud activation properties of aerosol particles in a continental Central European urban environment

2021 ◽  
Vol 21 (14) ◽  
pp. 11289-11302
Author(s):  
Imre Salma ◽  
Wanda Thén ◽  
Máté Vörösmarty ◽  
András Zénó Gyöngyösi
Keyword(s):  
Chemical Composition ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Aerosol Particles ◽  
Number Concentration ◽  
Urban Aerosol ◽  
Condensation Nuclei ◽  
Frequency Distributions ◽  
Remote Locations ◽  
Cloud Activation

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.

scholarly journals Measured and modelled Cloud Condensation Nuclei (CCN) concentration in São Paulo, Brazil: the importance of aerosol size-resolved chemical composition on CCN concentration prediction

2013 ◽  
Vol 13 (12) ◽  
pp. 32353-32389 ◽  
Author(s):  
G. P. Almeida ◽  
J. Brito ◽  
C. A. Morales ◽  
M. F. Andrade ◽  
P. Artaxo
Keyword(s):  
Chemical Composition ◽  
Real Time ◽  
Cloud Condensation Nuclei ◽  
Bulk Composition ◽  
Sao Paulo ◽  
Aerosol Size Distribution ◽  
São Paulo ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
The Impact

Abstract. Measurements of cloud condensation nuclei (CCN), aerosol size distribution and non-refractory chemical composition were performed from 16 to 31 October 2012 in the São Paulo Metropolitan Area (SPMA), Brazil. CCN measurements were performed at 0.2%, 0.4%, 0.6%, 0.8% and 1.0% water supersaturation and were subsequently compared with Köhler theory, considering the chemical composition. Real-time chemical composition has been obtained deploying for the first time in SPMA an Aerosol Chemical Ionization Monitor (ACSM). CCN closure analyses were performed considering internal mixture. Average aerosol composition during the studied period yielded 4.81 ± 3.05, 3.26 ± 2.10, 0.30 ± 0.27, 0.52 ± 0.32, 0.37 ± 0.21 and 0.04 ± 0.04 μg m−3 for organics, BC, NH4, SO4, NO3 and Cl, respectively. Particle number concentration was 12 813 ± 5350 cm−3, being a large fraction in the nucleation mode. CCN concentrations were on average 1090 ± 328 cm−3 and 3570 ± 1695 cm−3 at SS = 0.2% and SS = 1.0%, respectively. Results show an increase in aerosol hygroscopicity in the afternoon as a result of aerosol photochemical processing, leading to an enhancement of both organic and inorganic secondary aerosols in the atmosphere, as well as an increase in aerosol average diameter. Considering the bulk composition alone, CCN concentrations were substantially overpredicted (29.6 ± 45.1% at 0.2% supersaturation and 57.3 ± 30.0% at 1.0% supersaturation). Overall, the impact of composition on the calculated NCCN decreases with decreasing supersaturation, partially because using bulk composition introduces less bias for large diameters and lower critical supersaturations. Results suggest that the consideration of only inorganic fraction improves the calculated NCCN. Introducing a size-dependent chemical composition based on filter measurements from previous campaigns has considerably improved simulated values for NCCN (average overprediction error 3.0 ± 33.4% at 0.20% supersaturation and average under prediction error 2.4 ± 20.5% at 1.0% supersaturation). This study provides the first insight on aerosol real-time composition and hygroscopicity on a~site strongly impacted by emissions of a unique vehicular fleet due to the extensive biofuel usage.

scholarly journals Hygroscopic properties and cloud condensation nuclei activity of atmospheric aerosols under the influences of Asian continental outflow and new particle formation at a coastal site in eastern Asia

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
Keyword(s):  
Chemical Composition ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
Number Concentration ◽  
Pollution Sources ◽  
New Particle Formation ◽  
Condensation Nuclei ◽  
Air Masses ◽  
Hygroscopic Properties ◽  
Aerosol Hygroscopicity

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.

scholarly journals Measured and modelled cloud condensation nuclei (CCN) concentration in São Paulo, Brazil: the importance of aerosol size-resolved chemical composition on CCN concentration prediction

2014 ◽  
Vol 14 (14) ◽  
pp. 7559-7572 ◽  
Author(s):  
G. P. Almeida ◽  
J. Brito ◽  
C. A. Morales ◽  
M. F. Andrade ◽  
P. Artaxo
Keyword(s):  
Chemical Composition ◽  
Real Time ◽  
Cloud Condensation Nuclei ◽  
Bulk Composition ◽  
Sao Paulo ◽  
Aerosol Size Distribution ◽  
São Paulo ◽  
Condensation Nuclei ◽  
Kohler Theory ◽  
The Impact

Abstract. Measurements of cloud condensation nuclei (CCN), aerosol size distribution and non-refractory chemical composition were performed from 16 to 31 October 2012 in the São Paulo Metropolitan Area (SPMA), Brazil. CCN measurements were performed at 0.23, 0.45, 0.68, 0.90 and 1.13% water supersaturation and were subsequently compared with the Köhler theory, considering the chemical composition. Real-time chemical composition has been obtained by deploying, for the first time in the SPMA, an aerosol chemical ionization monitor (ACSM). CCN closure analyses were performed considering internal mixtures. Average aerosol composition during the studied period yielded (arithmetic mean~± standard deviation) 4.81 ± 3.05, 3.26 ± 2.10, 0.30 ± 0.27, 0.52 ± 0.32, 0.37 ± 0.21 and 0.04 ± 0.04 μg m−3 for organics, BC, NH4, SO4, NO3 and Cl, respectively. Particle number concentration was 12 813 ± 5350 cm−3, with a dominant nucleation mode. CCN concentrations were on average 1090 ± 328 and 3570 ± 1695 cm−3 at SS = 0.23% and SS = 1.13%, respectively. Results show an increase in aerosol hygroscopicity in the afternoon as a result of aerosol photochemical processing, leading to an enhancement of both organic and inorganic secondary aerosols in the atmosphere, as well as an increase in aerosol average diameter. Considering the bulk composition alone, observed CCN concentrations were substantially overpredicted when compared with the Köhler theory (44.1 ± 47.9% at 0.23% supersaturation and 91.4 ± 40.3% at 1.13% supersaturation). Overall, the impact of composition on the calculated CCN concentration (NCCN) decreases with decreasing supersaturation, partially because using bulk composition introduces less bias for large diameters and lower critical supersaturations, defined as the supersaturation at which the cloud droplet activation will take place. Results suggest that the consideration of only inorganic fraction improves the calculated NCCN. Introducing a size-dependent chemical composition based on filter measurements from previous campaigns has considerably improved simulated values for NCCN (average overprediction error 14.8 ± 38.6% at 0.23% supersaturation and 3.6 ± 21.6% at 1.13% supersaturation). This study provides the first insight on aerosol real-time composition and hygroscopicity at a site strongly impacted by emissions of a unique vehicular fleet due to the extensive biofuel usage.

scholarly journals Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing

2018 ◽  
Vol 18 (9) ◽  
pp. 6907-6921 ◽  
Author(s):  
Jingye Ren ◽  
Fang Zhang ◽  
Yuying Wang ◽  
Don Collins ◽  
Xinxin Fan ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Black Carbon ◽  
Cloud Condensation Nuclei ◽  
Field Measurements ◽  
Minor Role ◽  
Mixing State ◽  
Mixing Processes ◽  
Size Dependent ◽  
Aerosol Mixing State ◽  
Aerosol Chemical Composition

Abstract. Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (NCCN). In this study, we predict NCCN under five assumed schemes of aerosol chemical composition and mixing state based on field measurements in Beijing during the winter of 2016. Our results show that the best closure is achieved with the assumption of size dependent chemical composition for which sulfate, nitrate, secondary organic aerosols, and aged black carbon are internally mixed with each other but externally mixed with primary organic aerosol and fresh black carbon (external–internal size-resolved, abbreviated as EI–SR scheme). The resulting ratios of predicted-to-measured NCCN (RCCN_p∕m) were 0.90 – 0.98 under both clean and polluted conditions. Assumption of an internal mixture and bulk chemical composition (INT–BK scheme) shows good closure with RCCN_p∕m of 1.0 –1.16 under clean conditions, implying that it is adequate for CCN prediction in continental clean regions. On polluted days, assuming the aerosol is internally mixed and has a chemical composition that is size dependent (INT–SR scheme) achieves better closure than the INT–BK scheme due to the heterogeneity and variation in particle composition at different sizes. The improved closure achieved using the EI–SR and INT–SR assumptions highlight the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. NCCN is significantly underestimated (with RCCN_p∕m of 0.66 – 0.75) when using the schemes of external mixtures with bulk (EXT–BK scheme) or size-resolved composition (EXT–SR scheme), implying that primary particles experience rapid aging and physical mixing processes in urban Beijing. However, our results show that the aerosol mixing state plays a minor role in CCN prediction when the κorg exceeds 0.1.

scholarly journals The influence of chemical composition and mixing state of Los Angeles urban aerosol on CCN number and cloud properties

2008 ◽  
Vol 8 (18) ◽  
pp. 5649-5667 ◽  
Author(s):  
M. J. Cubison ◽  
B. Ervens ◽  
G. Feingold ◽  
K. S. Docherty ◽  
I. M. Ulbrich ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Los Angeles ◽  
Cloud Condensation Nuclei ◽  
Number Concentration ◽  
The State ◽  
Urban Aerosol ◽  
Mixing State ◽  
Data Set ◽  
Hygroscopic Properties ◽  
Aerosol Distribution

Abstract. The relationship between cloud condensation nuclei (CCN) number and the physical and chemical properties of the atmospheric aerosol distribution is explored for a polluted urban data set from the Study of Organic Aerosols at Riverside I (SOAR-1) campaign conducted at Riverside, California, USA during summer 2005. The mixing state and, to a lesser degree, the average chemical composition are shown to be important parameters in determining the activation properties of those particles around the critical activation diameters for atmospherically-realistic supersaturation values. Closure between predictions and measurements of CCN number at several supersaturations is attempted by modeling a number of aerosol chemical composition and mixing state cases of increasing complexity. It is shown that a realistic treatment of the state of mixing of the urban aerosol distribution is critical in order to eliminate model bias. Fresh emissions such as elemental carbon and small organic particles must be treated as non-activating and explicitly accounted for in the model. The relative number concentration of these particles compared to inorganics and oxygenated organic compounds of limited hygroscopicity plays an important role in determining the CCN number. Furthermore, expanding the different composition/mixing state cases to predictions of cloud droplet number concentration in a cloud parcel model highlights the dependence of cloud optical properties on the state of mixing and hygroscopic properties of the different aerosol modes, but shows that the relative differences between the different cases are reduced compared to those from the CCN model.

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