scholarly journals Organic acids as cloud condensation nuclei: Laboratory studies of highly soluble and insoluble species

2003 ◽  
Vol 3 (1) ◽  
pp. 949-982 ◽  
Author(s):  
P. Pradeep Kumar ◽  
K. Broekhuizen ◽  
J. P. D. Abbatt
Keyword(s):  
Organic Acids ◽  
Room Temperature ◽  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Diffusion Chamber ◽  
Laboratory Studies ◽  
Condensation Nuclei ◽  
Gradient Diffusion ◽  
Kohler Theory ◽  
Good Agreement

Abstract. The ability of sub-micron-sized organic acid particles to act as cloud condensation nuclei (CCN) has been examined at room temperature using a newly constructed continuous-flow, thermal-gradient diffusion chamber (TGDC). The organic acids studied were: oxalic, malonic, glutaric, oleic and stearic. The CCN properties of the highly soluble acids – oxalic, malonic and glutaric – match very closely Kohler theory predictions which assume full dissolution of the dry particle and a surface tension of the growing droplet equal to that of water. In particular, for supersaturations between 0.3 and 0.6, agreement between the dry particle diameter which gives 50% activation and that calculated from Kohler theory is to within 3 nm on average. In the course of the experiments, considerable instability of glutaric acid particles was observed as a function of time and there is evidence that they fragment to some degree to smaller particles. Stearic acid and oleic acid, which are both highly insoluble in water, did not activate at supersaturations of 0.6% with dry diameters up to 140 nm. Finally, to validate the performance of the TGDC, we present results for the activation of ammonium sulfate particles that demonstrate good agreement with Kohler theory if solution non-ideality is considered. Our findings support earlier studies in the literature that showed highly soluble organics to be CCN active but insoluble species to be largely inactive.

scholarly journals Organic acids as cloud condensation nuclei: Laboratory studies of highly soluble and insoluble species

2003 ◽  
Vol 3 (3) ◽  
pp. 509-520 ◽  
Author(s):  
P. Pradeep Kumar ◽  
K. Broekhuizen ◽  
J. P. D. Abbatt
Keyword(s):  
Organic Acids ◽  
Room Temperature ◽  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Diffusion Chamber ◽  
Laboratory Studies ◽  
Condensation Nuclei ◽  
Gradient Diffusion ◽  
Kohler Theory ◽  
Good Agreement

Abstract. The ability of sub-micron-sized organic acid particles to act as cloud condensation nuclei (CCN) has been examined at room temperature using a newly constructed continuous-flow, thermal-gradient diffusion chamber (TGDC). The organic acids studied were: oxalic, malonic, glutaric, oleic and stearic. The CCN properties of the highly soluble acids - oxalic, malonic and glutaric - match very closely Köhler theory predictions which assume full dissolution of the dry particle and a surface tension of the growing droplet equal to that of water. In particular, for supersaturations between 0.3 and 0.6, agreement between the dry particle diameter which gives 50% activation and that calculated from Köhler theory is to within 3nm on average. In the course of the experiments, considerable instability of glutaric acid particles was observed as a function of time and there is evidence that they fragment to some degree to smaller particles. Stearic acid and oleic acid, which are both highly insoluble in water, did not activate at supersaturations of 0.6% with dry diameters up to 140nm. Finally, to validate the performance of the TGDC, we present results for the activation of ammonium sulfate particles that demonstrate good agreement with Köhler theory if solution non-ideality is considered. Our findings support earlier studies in the literature that showed highly soluble organics to be CCN active but insoluble species to be largely inactive.

scholarly journals Closure between measured and modeled cloud condensation nuclei (CCN) using size-resolved aerosol compositions in downtown Toronto

2005 ◽  
Vol 5 (4) ◽  
pp. 6263-6293 ◽  
Author(s):  
K. Broekhuizen ◽  
R. Y.-W. Chang ◽  
W. R. Leaitch ◽  
S.-M. Li ◽  
J. P. D. Abbatt
Keyword(s):  
Cloud Condensation Nuclei ◽  
Compositional Analysis ◽  
Diffusion Chamber ◽  
Aerosol Size Distribution ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
Average Value ◽  
Aerosol Mass ◽  
Gradient Diffusion ◽  
Kohler Theory

Abstract. Measurements of cloud condensation nuclei (CCN) were made in downtown Toronto during August and September, 2003. CCN measurements were performed at 0.58% supersaturation using a thermal-gradient diffusion chamber, whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and APS system and an Aerodyne Aerosol Mass Spectrometer (AMS), respectively. Aerosol composition data shows that the particles were predominately organic in nature, in particular for those with a vacuum aerodynamic diameter of <25 μm. In this study, the largest contribution to CCN concentrations came from this size range, suggesting that the CCN are also organic-rich. Using the size and composition information, a detailed CCN closure analysis was performed. In all analyses, the particles were assumed to be internally mixed, the organic fraction was assumed to be insoluble, and the inorganic fraction was assumed to be ammonium sulfate. The AMS time-of-flight data were used for Köhler theory predictions for each particle size and composition to obtain the dry diameter required for activation. By so doing, this closure analysis yielded an average value of CCNpredicted/CCNobserved= 1.04 (R2=0.87). Several other closure analyses were performed to mimic other methods of aerosol compositional analysis. In all cases, by assuming uniform aerosol composition across a wider range of particle sizes, significant overprediction of CCN concentrations resulted.

scholarly journals Closure between measured and modeled cloud condensation nuclei (CCN) using size-resolved aerosol compositions in downtown Toronto

2006 ◽  
Vol 6 (9) ◽  
pp. 2513-2524 ◽  
Author(s):  
K. Broekhuizen ◽  
R.Y.-W. Chang ◽  
W. R. Leaitch ◽  
S.-M. Li ◽  
J. P. D. Abbatt
Keyword(s):  
Cloud Condensation Nuclei ◽  
Diffusion Chamber ◽  
Droplet Surface ◽  
Aerosol Size Distribution ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
Average Value ◽  
Aerosol Mass ◽  
Gradient Diffusion ◽  
Kohler Theory

Abstract. Measurements of cloud condensation nuclei (CCN) were made in downtown Toronto during August and September, 2003. CCN measurements were performed at 0.58% supersaturation using a thermal-gradient diffusion chamber, whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and APS system and an Aerodyne Aerosol Mass Spectrometer (AMS), respectively. Aerosol composition data shows that the particles were predominately organic in nature, in particular for those with a vacuum aerodynamic diameter of <0.25 µm. In this study, the largest contribution to CCN concentrations came from this size range, suggesting that the CCN are also organic-rich. Using the size and composition information, detailed CCN closure analyses were performed. In the first analysis, the particles were assumed to be internally mixed, the organic fraction was assumed to be insoluble, and the inorganic fraction was assumed to be ammonium sulfate. The AMS time-of-flight data were used for Köhler theory predictions for each particle size and composition to obtain the dry diameter required for activation. By so doing, this closure analysis yielded an average value of CCNpredicted/CCNobserved=1.12±0.05. However, several sample days showed distinct bimodal distributions, and a closure analysis was performed after decoupling the two particle modes. This analysis yielded an average value of CCNpredicted/CCNobserved=1.03±0.05. A sensitivity analysis was also performed to determine the aerosol/CCN closure if the organic solubility, droplet surface tension, or chamber supersaturation were varied.

scholarly journals Summertime observations of ultrafine particles and cloud condensation nuclei from the boundary layer to the free troposphere in the Arctic

2016 ◽  
Author(s):  
Julia Burkart ◽  
Megan D. Willis ◽  
Heiko Bozem ◽  
Jennie L. Thomas ◽  
Kathy Law ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Ultrafine Particles ◽  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Open Ocean ◽  
The Arctic ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
Low Level ◽  
20 Nm

Abstract. The Arctic is extremely sensitive to climate change. Shrinking sea ice extent increases the area covered by open ocean during Arctic summer, which impacts the surface albedo and aerosol and cloud properties among many things. In this context extensive aerosol measurements (aerosol composition, particle number and size, cloud condensation nuclei, and trace gases) were made during 11 flights of the NETCARE July, 2014 airborne campaign conducted from Resolute Bay, Nunavut (74N, 94W). Flights routinely included vertical profiles from about 60 to 3000 m a.g.l. as well as several low-level horizontal transects over open ocean, fast ice, melt ponds, and polynyas. Here we discuss the vertical distribution of ultrafine particles (UFP, particle diameter, dp: 5–20 nm), size distributions of larger particles (dp: 20 nm to 1 μm), and cloud condensation nuclei (CCN, supersaturation = 0.6 %) in relation to meteorological conditions and underlying surfaces. UFPs were observed predominantly within the boundary layer, where concentrations were often several hundreds to a few thousand particles per cubic centimeter. Occasionally, particle concentrations below 10 cm−3 were found. The highest UFP concentrations were observed above open ocean and at the top of low-level clouds, whereas numbers over ice-covered regions were substantially lower. Overall, UFP formation events were frequent in a clean boundary layer with a low condensation sink. In a few cases this ultrafine mode extended to sizes larger than 40 nm, suggesting that these UFP can grow into a size range where they can impact clouds and therefore climate.

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 Technical note: Characterization of a static thermal-gradient CCN counter

2006 ◽  
Vol 6 (2) ◽  
pp. 2151-2174 ◽  
Author(s):  
G. P. Frank ◽  
U. Dusek ◽  
M. O. Andreae
Keyword(s):  
Water Vapor ◽  
Thermal Gradient ◽  
Cloud Condensation Nuclei ◽  
Diffusion Chamber ◽  
Calibration Method ◽  
Theoretical Description ◽  
Technical Note ◽  
Number Concentration ◽  
Gradient Diffusion

Abstract. The static (parallel-plate thermal-gradient) diffusion chamber (SDC) was one of the first instruments designed to measure cloud condensation nuclei (CCN) concentrations as a function of supersaturation. It has probably also been the most widely used type of CCN counter. This paper describes the detailed experimental characterization of a SDC CCN counter, including calibration with respect to supersaturation and particle number concentration. In addition, we investigated the proposed effect of lowered supersaturation because of water vapor depletion with increasing particle concentration. The results obtained gives a larger understanding why and in which way it is necessary to calibrate the SDC CCN counter. The calibration method is described in detail as well. The method can, in parts, be used for calibrations also for other types of CCN counters. We conclude the following: 1) it is important to experimentally calibrate SDC CCN counters with respect to supersaturation, and not only base the supersaturation on the theoretical description of the instrument; 2) the number concentration calibration needs to be performed as a function of supersaturation, also for SDC CCN counter using the photographic technique; and 3) we observed no evidence that water vapor depletion lowered the supersaturation.

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 Cloud droplet activity changes of soot aerosol upon smog chamber ageing

2014 ◽  
Vol 14 (18) ◽  
pp. 9831-9854 ◽  
Author(s):  
C. Wittbom ◽  
A. C. Eriksson ◽  
J. Rissler ◽  
J. E. Carlsson ◽  
P. Roldin ◽  
...  
Keyword(s):  
Uv Radiation ◽  
Organic Material ◽  
Mass Fraction ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Particle Morphology ◽  
Organic Aerosol ◽  
Condensation Nuclei ◽  
Soot Particles ◽  
Kohler Theory

Abstract. Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤2%, i.e. the BC core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatility organic compounds (IVOCs) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (e.g. primary or secondary organic aerosol), (III) particle size, and (IV) particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input parameters describing the organic material), showed good agreement with cloud droplet activation measurements for particles with a SOA mass fraction ≥0.12 (slightly aged particles). The activation properties are enhanced with only a slight increase in organic material coating the soot particles (SOA mass fraction < 0.12), however not as much as predicted by Köhler theory. The discrepancy between theory and experiments during the early stages of ageing might be due to solubility limitations, unevenly distributed organic material or hindering particle morphology. The change in properties of soot nanoparticles upon photochemical processing clearly increases their hygroscopicity, which affects their behaviour both in the atmosphere and in the human respiratory system.

scholarly journals Physical properties of the sub-micrometer aerosol over the Amazon rain forest during the wet-to-dry season transition - comparison of modeled and measured CCN concentrations

2004 ◽  
Vol 4 (8) ◽  
pp. 2119-2143 ◽  
Author(s):  
J. Rissler ◽  
E. Swietlicki ◽  
J. Zhou ◽  
G. Roberts ◽  
M. O. Andreae ◽  
...  
Keyword(s):  
Size Distribution ◽  
Biomass Burning ◽  
Time Resolution ◽  
Large Scale ◽  
Transition Period ◽  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Hygroscopic Growth ◽  
Condensation Nuclei ◽  
Number Size Distribution

Abstract. Sub-micrometer atmospheric aerosol particles were studied in the Amazon region, 125 km northeast of Manaus, Brazil (-1°55.2'S, 59°28.1'W). The measurements were performed during the wet-to-dry transition period, 4-28 July 2001 as part of the LBA (Large-Scale Biosphere Atmosphere Experiment in Amazonia) CLAIRE-2001 (Cooperative LBA Airborne Regional Experiment) experiment. The number size distribution was measured with two parallel differential mobility analyzers, the hygroscopic growth at 90% RH with a Hygroscopic Tandem Mobility Analyzer (H-TDMA) and the concentrations of cloud condensation nuclei (CCN) with a cloud condensation nuclei counter. A model was developed that uses the H-TDMA data to predict the number of soluble molecules or ions in the individual particles and the corresponding minimum particle diameter for activation into a cloud droplet at a certain supersaturation. Integrating the number size distribution above this diameter, CCN concentrations were predicted with a time resolution of 10 min and compared to the measured concentrations. During the study period, three different air masses were identified and compared: clean background, air influenced by aged biomass burning, and moderately polluted air from recent local biomass burning. For the clean period 2001, similar number size distributions and hygroscopic behavior were observed as during the wet season at the same site in 1998, with mostly internally mixed particles of low diameter growth factor (~1.3 taken from dry to 90% RH). During the periods influenced by biomass burning the hygroscopic growth changed slightly, but the largest difference was seen in the number size distribution. The CCN model was found to be successful in predicting the measured CCN concentrations, typically within 25%. A sensitivity study showed relatively small dependence on the assumption of which model salt that was used to predict CCN concentrations from H-TDMA data. One strength of using H-TDMA data to predict CCN concentrations is that the model can also take into account soluble organic compounds, insofar as they go into solution at 90% RH. Another advantage is the higher time resolution compared to using size-resolved chemical composition data.

Sign in / Sign up

Export Citation Format

Share Document