scholarly journals Establishing the Impact of Model Surfactants on Cloud Condensation Nuclei Activity of Sea Spray Aerosols

2018 ◽  
Author(s):  
Sara D. Forestieri ◽  
Sean M. Staudt ◽  
Thomas M. Kuborn ◽  
Katharine Faber ◽  
Christopher R. Ruehl ◽  
...  
Keyword(s):  
Surface Tension ◽  
Oleic Acid ◽  
Palmitic Acid ◽  
Water Uptake ◽  
Myristic Acid ◽  
Cloud Condensation Nuclei ◽  
Sea Spray ◽  
Condensation Nuclei ◽  
Molecular Area ◽  
The Impact

Abstract. Surface active compounds present in aerosols can increase their cloud condensation nuclei (CCN) activation efficiency by reducing the surface tension (σ) in the growing droplets. However, the importance of this effect is poorly constrained by measurements. Here we present estimates of droplet surface tension near the point of activation derived from direct measurement of droplet diameters using a continuous flow stream-wise thermal gradient chamber (CFSTGC). The experiments used sea spray aerosol mimics composed of NaCl coated by varying amounts of (i) oleic acid, palmitic acid or myristic acid, (ii) mixtures of palmitic acid and oleic acid, and (iii) oxidized oleic acid. Significant reductions in σ relative to that for pure water were observed for these mimics at relative humidity (RH) near activation (~ 99.9 %) when the coating was sufficiently thick. The calculated surface pressure (π = σH2O − σobserved) values for a given organic compound or mixture collapse onto one curve when plotted as a function of molecular area for different NaCl seed sizes and measured RH. The observed critical molecular area (A0) for oleic acid determined from droplet growth was similar to that from bulk experiments conducted in a Langmuir trough. However, the observations presented here suggest that oleic acid in microscopic droplets may exhibit larger π values during monolayer compression. For myristic acid, the observed A0 compared well to bulk experiments on a fresh subphase, for which dissolution has an important impact. A significant kinetic limitation to water uptake was observed for NaCl particles coated with pure palmitic acid, likely as a result of palmitic acid being able to form a solid film. However, for binary palmitic acid-oleic acid mixtures there was no evidence of a kinetic limitation to water uptake. Oxidation of oleic acid had a minor impact on the magnitude of the surface tension reductions observed, potentially leading to a slight reduction in the effect compared to pure oleic acid. A cloud condensation nuclei (CCN) counter was also used to assess the impact on critical supersaturations of the substantial σ reductions observed at very high RH. For the fatty acid-coated NaCl particles, when the organic fraction (εorg) was > 0.90 small depressions in critical supersaturation were observed. However, when εorg 

scholarly journals Establishing the impact of model surfactants on cloud condensation nuclei activity of sea spray aerosol mimics

2018 ◽  
Vol 18 (15) ◽  
pp. 10985-11005 ◽  
Author(s):  
Sara D. Forestieri ◽  
Sean M. Staudt ◽  
Thomas M. Kuborn ◽  
Katharine Faber ◽  
Christopher R. Ruehl ◽  
...  
Keyword(s):  
Surface Tension ◽  
Oleic Acid ◽  
Palmitic Acid ◽  
Organic Molecules ◽  
Cloud Condensation Nuclei ◽  
Critical Supersaturation ◽  
Activation Efficiency ◽  
Sea Spray Aerosol ◽  
Surface Active ◽  
The Impact

Abstract. Surface-active compounds present in aerosols can increase their cloud condensation nuclei (CCN) activation efficiency by reducing the surface tension (σ) in the growing droplets. However, the importance of this effect is poorly constrained by measurements. Here we present estimates of droplet surface tension near the point of activation derived from direct measurement of droplet diameters using a continuous flow streamwise thermal gradient chamber (CFSTGC). The experiments used sea spray aerosol (SSA) mimics composed of NaCl coated by varying amounts of (i) oleic acid, palmitic acid or myristic acid, (ii) mixtures of palmitic acid and oleic acid, and (iii) oxidized oleic acid. Significant reductions in σ relative to that for pure water were observed for these mimics at relative humidity (RH) near activation (∼ 99.9 %) when the coating was sufficiently thick. The calculated surface pressure (π = σH2O − σobserved) values for a given organic compound or mixture collapse onto one curve when plotted as a function of molecular area for different NaCl seed sizes and measured RH. The observed critical molecular area (A0) for oleic acid determined from droplet growth was similar to that from experiments conducted using macroscopic solutions in a Langmuir trough. However, the observations presented here suggest that oleic acid in microscopic droplets may exhibit larger π values during monolayer compression. For myristic acid, the observed A0 compared well to macroscopic experiments on a fresh subphase, for which dissolution has an important impact. A significant kinetic limitation to water uptake was observed for NaCl particles coated with pure palmitic acid, likely as a result of palmitic acid (with coating thicknesses ranging from 67 to 132 nm) being able to form a solid film. However, for binary palmitic-acid–oleic-acid mixtures there was no evidence of a kinetic limitation to water uptake. Oxidation of oleic acid had a minor impact on the magnitude of the surface tension reductions observed, potentially leading to a slight reduction in the effect compared to pure oleic acid. A CCN counter was also used to assess the impact on critical supersaturations of the substantial σ reductions observed at very high RH. For the fatty-acid-coated NaCl particles, when the organic fraction (εorg) was > 0.90 small depressions in critical supersaturation were observed. However, when εorg < 0.90 the impact on critical supersaturation was negligible. Thus, for the fatty acids considered here, the substantial σ reductions observed at high RH values just below activation have limited impact on the ultimate critical supersaturation. A surface film model is used to establish the properties that surface-active organic molecules must have if they are to ultimately have a substantial impact on the activation efficiency of SSA. To influence activation, the average properties of surface-active marine-derived organic molecules must differ substantially from the long-chain fatty acids examined, having either smaller molecular volumes or larger molecular areas. The model results also indicate that organic-compound-driven surface tension depression can serve to buffer the critical supersaturation against changes to the organic-to-salt ratio in particles in which the organic fraction is sufficiently large.

scholarly journals Effect of primary organic sea spray emissions on cloud condensation nuclei concentrations

2011 ◽  
Vol 11 (2) ◽  
pp. 5757-5784 ◽  
Author(s):  
D. M. Westervelt ◽  
R. H. Moore ◽  
A. Nenes ◽  
P. J. Adams
Keyword(s):  
Surface Tension ◽  
General Circulation ◽  
Source Function ◽  
Cloud Condensation Nuclei ◽  
Organic Aerosol ◽  
Biologically Active ◽  
Sea Spray ◽  
Condensation Nuclei ◽  
Aerosol Emission ◽  
Surfactant Effects

Abstract. This work quantifies the primary marine organic aerosol global emission source and its impact on cloud condensation nuclei (CCN) concentrations by implementing an organic sea spray source function into a series of global aerosol simulations. The source function assumes that a fraction of the sea spray emissions, depending on the local chlorophyll concentration, is organic matter in place of NaCl. Effect on CCN concentrations (at 0.2% supersaturation) is modeled using the Two-Moment Aerosol Sectional (TOMAS) microphysics algorithm coupled to the GISS II-prime general circulation model. The presence of organics affects CCN activity in competing ways: by reducing the amount of solute available in the particle and decreasing surface tension of CCN. To model surfactant effects, surface tension depression data from seawater samples taken near the Georgia coast were applied as a function of carbon concentrations. A global marine organic aerosol emission rate of 17.7 Tg C yr−1 is estimated from the simulations. Marine organics exert a localized influence on CCN(0.2%) concentrations, decreasing regional concentrations by no more than 5% and by less than 0.5% over most of the globe. The decrease in CCN concentrations results from the fact that the decrease in particle solute concentration outweighs the organic surfactant effects. The low sensitivity of CCN(0.2%) to the marine organic emissions is likely due to the small compositional changes: the mass fraction of OA in accumulation mode aerosol increases by only 15% in a biologically active region of the Southern Ocean.

scholarly journals Supplementary material to "Establishing the Impact of Model Surfactants on Cloud Condensation Nuclei Activity of Sea Spray Aerosols"

2018 ◽  
Author(s):  
Sara D. Forestieri ◽  
Sean M. Staudt ◽  
Thomas M. Kuborn ◽  
Katharine Faber ◽  
Christopher R. Ruehl ◽  
...  
Keyword(s):  
Cloud Condensation Nuclei ◽  
Sea Spray ◽  
Condensation Nuclei ◽  
Supplementary Material ◽  
The Impact

New Directions: The impact of oceanic iron fertilisation on cloud condensation nuclei

2008 ◽  
Vol 42 (22) ◽  
pp. 5728-5730 ◽  
Author(s):  
Matthew T. Woodhouse ◽  
Graham W. Mann ◽  
Kenneth S. Carslaw ◽  
Olivier Boucher
Keyword(s):  
Cloud Condensation Nuclei ◽  
Condensation Nuclei ◽  
New Directions ◽  
The Impact

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 Sensitivity Studies on the Impact of Dust and Aerosol Pollution Acting as Cloud Nucleating Aerosol on Orographic Precipitation in the Colorado River Basin

2018 ◽  
Vol 2018 ◽  
pp. 1-15 ◽  
Author(s):  
Vandana Jha ◽  
William R. Cotton ◽  
Gustavo G. Carrió ◽  
Robert Walko
Keyword(s):  
River Basin ◽  
Colorado River ◽  
Cloud Condensation Nuclei ◽  
Winter Season ◽  
Colorado River Basin ◽  
Orographic Precipitation ◽  
Condensation Nuclei ◽  
Aerosol Pollution ◽  
Sensitivity Studies ◽  
The Impact

In this study, we examine the cumulative effect of pollution aerosol and dust acting as cloud nucleating aerosol;cloud condensation nuclei (CCN), giant cloud condensation nuclei, and ice nuclei (IN), on orographic precipitation in the Rocky Mountains. We analyze the results of sensitivity studies for specific cases in 2004-2005 winter season to analyze the relative impact of aerosol pollution and dust acting as CCN and IN on precipitation in the Colorado River Basin. Dust is varied from 3 to 10 times in the experiments, and the response is found to be nonmonotonic and depends on various environmental factors. The sensitivity studies show that adding dust in a wet system increases precipitation when IN effects are dominant. For a relatively dry system high concentrations of dust can result in overseeding the clouds and reductions in precipitation. However, when adding dust to a system with warmer cloud bases where drizzle formation is active, the response is nonmonotonic.

Acoustic Cloud Condensation Nuclei Counter

2005 ◽  
Author(s):  
Abhijit Deshpande ◽  
Marcellin Zahui
Keyword(s):  
Water Surface ◽  
Cloud Condensation Nuclei ◽  
Droplet Diameter ◽  
Bubble Formation ◽  
Maximum Velocity ◽  
Acoustic Energy ◽  
Water Droplets ◽  
Condensation Nuclei ◽  
Micro Scale ◽  
The Impact

Analysis and simulation of an acoustic cloud condensation nuclei counter is presented. The instrument is capable of accurately counting the number of micro scale water droplets impacting a water surface. The sound produced underwater by the water droplets is determined when the droplets strike the water surface with an impact velocity equal to either their terminal or maximum velocity. First, the terminal velocities of the droplets are calculated using Stoke’s law and compared to measured velocities from Gunn and Kinzer. Then the maximum velocities that these droplets can sustain without breaking are calculated as a function of droplet diameter. Second, the sound due to droplet impact is estimated. Due to their size and water surface tension, there is no bubble formation at impact when the droplets are falling with terminal velocities. However conditions for regular bubble entrainments are established and limit velocities are calculated. Assuming that the micro water droplets can be accelerated, the maximum velocities for no bubble entrainments are calculated. The results show that the level of the sound produced by individual micro scale droplet falling with terminal velocity is so small that experimental verification is not possible. However, reasonable level of acoustic energy can be obtained by increasing the impact velocities of the droplets or by measuring the sound radiated by a group of impacting droplets. Finally, the droplets counting process is simulated using a water surface of one centimeter squared and a vertical growth chamber.

scholarly journals The relative impact of cloud condensation nuclei and ice nucleating particle concentrations on phase partitioning in Arctic mixed-phase stratocumulus clouds

2018 ◽  
Vol 18 (23) ◽  
pp. 17047-17059 ◽  
Author(s):  
Amy Solomon ◽  
Gijs de Boer ◽  
Jessie M. Creamean ◽  
Allison McComiskey ◽  
Matthew D. Shupe ◽  
...  
Keyword(s):  
Cloud Condensation Nuclei ◽  
Mixed Phase ◽  
Radiative Properties ◽  
Condensation Nuclei ◽  
Phase Partitioning ◽  
Cloud Dynamics ◽  
Stratocumulus Clouds ◽  
Cloud Ice ◽  
Mixed Phase Clouds ◽  
The Impact

Abstract. This study investigates the interactions between cloud dynamics and aerosols in idealized large-eddy simulations (LES) of Arctic mixed-phase stratocumulus clouds (AMPS) observed at Oliktok Point, Alaska, in April 2015. This case was chosen because it allows the cloud to form in response to radiative cooling starting from a cloud-free state, rather than requiring the cloud ice and liquid to adjust to an initial cloudy state. Sensitivity studies are used to identify whether there are buffering feedbacks that limit the impact of aerosol perturbations. The results of this study indicate that perturbations in ice nucleating particles (INPs) dominate over cloud condensation nuclei (CCN) perturbations; i.e., an equivalent fractional decrease in CCN and INPs results in an increase in the cloud-top longwave cooling rate, even though the droplet effective radius increases and the cloud emissivity decreases. The dominant effect of ice in the simulated mixed-phase cloud is a thinning rather than a glaciation, causing the mixed-phase clouds to radiate as a grey body and the radiative properties of the cloud to be more sensitive to aerosol perturbations. It is demonstrated that allowing prognostic CCN and INPs causes a layering of the aerosols, with increased concentrations of CCN above cloud top and increased concentrations of INPs at the base of the cloud-driven mixed layer. This layering contributes to the maintenance of the cloud liquid, which drives the dynamics of the cloud system.

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.

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