scholarly journals Impact of aerosol composition on cloud condensation nuclei activity

2012 ◽  
Vol 12 (1) ◽  
pp. 1493-1516
Author(s):  
Q. Zhang ◽  
J. Meng ◽  
J. Quan ◽  
Y. Gao ◽  
D. Zhao ◽  
...  
Keyword(s):  
Size Distribution ◽  
Field Experiments ◽  
Cloud Condensation Nuclei ◽  
Diffusion Chamber ◽  
Aerosol Size Distribution ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
Rate Of Increase ◽  
The Impact ◽  
Ccn Activity

Abstract. The impact of aerosol composition on cloud condensation nuclei (CCN) activity was analyzed in this study based on field experiments carried out at downtown Tianjin, China, in September 2010. In the experiments, the CCN measurements were performed at supersaturation (SS) of 0.1%, 0.2% and 0.4% using a thermal-gradient diffusion chamber (DMT CCNC), whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and an Aerodyne Aerosol Mass Spectrometer (AMS), respectively. The results show that the influence of aerosol composition on CCN activity is notable under low SS (0.1%), and their influence decreased with increasing SS. For example, under SS of 0.1%, the CCN activity increases from 4.5 ± 2.6% to 12.8 ± 6.1% when organics fraction decrease from 30–40% to 10–20%. The rate of increase reaches up to 184%. While under SS of 0.4%, the CCN activity increases only from 35.7 ± 19.0% to 46.5 ± 12.3%, correspondingly. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlates well with observed NCCN at high SS (0.4%), but this correlation decreases with the falling of SS. The slopes of linear fitted lines between calculated and observed NCCN are 0.708, 0.947, and 0.995 at SS of 0.1%, 0.2% and 0.4%, respectively. Moreover, the standard deviation (SD) of calculated NCCN increases with the decreasing of SS. A case study of CCN closure analyses indicates that the calculated error of NCCN can reach up to 34% at SS of 0.1% if aerosol composition is not included, and the calculated error decreases with the raising of SS. It decreases to 9% at SS of 0.2%, and further decreases to 4% at SS of 0.4%.

scholarly journals Impact of aerosol composition on cloud condensation nuclei activity

2012 ◽  
Vol 12 (8) ◽  
pp. 3783-3790 ◽  
Author(s):  
Q. Zhang ◽  
J. Meng ◽  
J. Quan ◽  
Y. Gao ◽  
D. Zhao ◽  
...  
Keyword(s):  
Size Distribution ◽  
Field Experiments ◽  
Cloud Condensation Nuclei ◽  
Diffusion Chamber ◽  
Aerosol Size Distribution ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
Rate Of Increase ◽  
The Impact ◽  
Ccn Activity

Abstract. The impact of aerosol composition on cloud condensation nuclei (CCN) activity were analyzed in this study based on field experiments carried out at downtown Tianjin, China in September 2010. In the experiments, the CCN measurements were performed at supersaturation (SS) of 0.1%, 0.2% and 0.4% using a thermal-gradient diffusion chamber (DMT CCNC), whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and an Aerodyne Aerosol Mass Spectrometer (AMS), respectively. The results show that the influence of aerosol composition on CCN activity is notable under low SS (0.1%), and their influence decreased with increasing SS. For example, under SS of 0.1%, the CCN activity increases from 4.5±2.6% to 12.8±6.1% when organics fraction decrease from 30–40% to 10–20%. The rate of increase reached up to 184%. While under SS of 0.4%, the CCN activity increases only from 35.7±19.0% to 46.5±12.3% correspondingly. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlated well with observed NCCN at high SS (0.4%), but this consistence decreased with the falling of SS. The slopes of linear fitted lines between calculated and observed NCCN are 0.708, 0.947, and 0.995 at SS of 0.1%, 0.2% and 0.4% respectively. Moreover, the stand deviation (SD) of calculated NCCN increased with the decreasing of SS. A case study of CCN closure analyses indicated that the calculated error of NCCN could reach up to 34% at SS of 0.1% if aerosol composition were not included, and the calculated error decreased with the raising of SS. It is decreased to 9% at SS of 0.2%, and further decreased to 4% at SS of 0.4%.

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 The role of the particle size distribution in assessing aerosol composition effects on simulated droplet activation

2010 ◽  
Vol 10 (2) ◽  
pp. 4189-4223 ◽  
Author(s):  
D. S. Ward ◽  
T. Eidhammer ◽  
W. R. Cotton ◽  
S. M. Kreidenweis
Keyword(s):  
Size Distribution ◽  
Cloud Condensation Nuclei ◽  
Atmospheric Modeling ◽  
Number Concentration ◽  
Aerosol Size Distribution ◽  
Detailed Knowledge ◽  
Aerosol Composition ◽  
Droplet Activation ◽  
The Impact ◽  
Aerosol Hygroscopicity

Abstract. Variations in the chemical composition of atmospheric aerosols alter their hygroscopicity and can lead to changes in the cloud-active fraction of the aerosols, or cloud condensation nuclei (CCN) number concentration. To investigate the importance of this effect under different atmospheric conditions, cloud droplet formation was simulated with a Lagrangian parcel model. Initial values of updraft speed and temperature were systematically varied along with aerosol number concentration, size and hygroscopicity (represented by the hygroscopicity parameter, κ). A previous study classifies the sensitivity of CCN activity to compositional changes based on the supersaturation reached in the parcel model. We found that these classifications could not be generalized to a range of aerosol size distribution median radii. Instead, variations in sensitivity with size depend on the location of the dry critical radius for droplet activation relative to the size distribution median radius. The parcel model output was used to construct droplet activation lookup tables based on κ that were implemented in the Regional Atmospheric Modeling System (RAMS) microphysical scheme. As a first application of this system, aerosol hygroscopicity and size were varied in a series of RAMS mesoscale simulations designed to investigate the sensitivity of a mixed-phase orographic cloud case to the parameter variations. Observations from a recent field campaign in northwestern Colorado provided the basis for the aerosol field initializations. Model results show moderate sensitivity in the distribution of total case precipitation to extreme changes in κ, and minimal sensitivity to observed changes in estimated κ. The impact of varying aerosol hygroscopicity diminished with increasing median radius, as expected from the parcel model results. The conclusions drawn from these simulations could simplify similar research in other cloud regimes by defining the need, or lack of need, for detailed knowledge of aerosol composition.

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 Aerosol size distribution seasonal characteristics measured in Tiksi, Russian Arctic

2015 ◽  
Vol 15 (13) ◽  
pp. 18109-18149 ◽  
Author(s):  
E. Asmi ◽  
V. Kondratyev ◽  
D. Brus ◽  
T. Laurila ◽  
H. Lihavainen ◽  
...  
Keyword(s):  
Size Distribution ◽  
Forest Fires ◽  
Cloud Condensation Nuclei ◽  
Source Region ◽  
Local Maximum ◽  
Aerosol Size Distribution ◽  
Aerosol Composition ◽  
Aerosol Sources ◽  
The Impact ◽  
Mass Concentrations

Abstract. Four years of continuous aerosol number size distribution measurements from an Arctic Climate Observatory in Tiksi Russia are analyzed. Source region effects on particle modal features, and number and mass concentrations are presented for different seasons. The monthly median total aerosol number concentration in Tiksi ranges from 184 cm-3 in November to 724 cm-3 in July with a local maximum in March of 481 cm-3. The total mass concentration has a distinct maximum in February–March of 1.72–2.38 μg m-3 and two minimums in June of 0.42 μg m-3 and in September–October of 0.36–0.57 μg m-3. These seasonal cycles in number and mass concentrations are related to isolated aerosol sources such as Arctic haze in early spring which increases accumulation and coarse mode numbers, and biogenic emissions in summer which affects the smaller, nucleation and Aitken mode particles. The impact of temperature dependent natural emissions on aerosol and cloud condensation nuclei numbers was significant. Therefore, in addition to the precursor emissions of biogenic volatile organic compounds, the frequent Siberian forest fires, although far are suggested to play a role in Arctic aerosol composition during the warmest months. During calm and cold months aerosol concentrations were occasionally increased by nearby aerosol sources in trapping inversions. These results provide valuable information on inter-annual cycles and sources of Arctic aerosols.

scholarly journals The role of the particle size distribution in assessing aerosol composition effects on simulated droplet activation

2010 ◽  
Vol 10 (12) ◽  
pp. 5435-5447 ◽  
Author(s):  
D. S. Ward ◽  
T. Eidhammer ◽  
W. R. Cotton ◽  
S. M. Kreidenweis
Keyword(s):  
Size Distribution ◽  
Cloud Condensation Nuclei ◽  
Atmospheric Modeling ◽  
Number Concentration ◽  
Aerosol Size Distribution ◽  
Detailed Knowledge ◽  
Aerosol Composition ◽  
Droplet Activation ◽  
The Impact ◽  
Aerosol Hygroscopicity

Abstract. Variations in the chemical composition of atmospheric aerosols alter their hygroscopicity and can lead to changes in the cloud-active fraction of the aerosols, or cloud condensation nuclei (CCN) number concentration. To investigate the importance of this effect under different atmospheric conditions, cloud droplet formation was simulated with a Lagrangian parcel model. Initial values of updraft speed and temperature were systematically varied along with aerosol number concentration, size and hygroscopicity (represented by the hygroscopicity parameter, κ). A previous study classifies the sensitivity of CCN activity to compositional changes based on the supersaturation reached in the parcel model. We found that these classifications could not be generalized to a range of aerosol size distribution median radii. Instead, variations in sensitivity with size depend on the location of the dry critical radius for droplet activation relative to the size distribution median radius. The parcel model output was used to construct droplet activation lookup tables based on κ that were implemented in the Regional Atmospheric Modeling System (RAMS) microphysical scheme. As a first application of this system, aerosol hygroscopicity and size were varied in a series of RAMS mesoscale simulations designed to investigate the sensitivity of a mixed-phase orographic cloud case to the parameter variations. Observations from a recent field campaign in northwestern Colorado provided the basis for the aerosol field initializations. Model results show moderate sensitivity in the distribution of total case precipitation to extreme changes in κ, and minimal sensitivity to observed changes in estimated κ. The impact of varying aerosol hygroscopicity diminished with increasing median radius, as expected from the parcel model results. The conclusions drawn from these simulations could simplify similar research in other cloud regimes by defining the need, or lack of need, for detailed knowledge of aerosol composition.

scholarly journals Prediction of cloud condensation nuclei activity for organic compounds using functional group contribution methods

2016 ◽  
Vol 9 (1) ◽  
pp. 111-124 ◽  
Author(s):  
M. D. Petters ◽  
S. M. Kreidenweis ◽  
P. J. Ziemann
Keyword(s):  
Organic Compounds ◽  
Field Experiments ◽  
Functional Group ◽  
Cloud Condensation Nuclei ◽  
Organic Aerosol ◽  
Group Contribution ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
Group Contribution Methods ◽  
Ccn Activity

Abstract. A wealth of recent laboratory and field experiments demonstrate that organic aerosol composition evolves with time in the atmosphere, leading to changes in the influence of the organic fraction to cloud condensation nuclei (CCN) spectra. There is a need for tools that can realistically represent the evolution of CCN activity to better predict indirect effects of organic aerosol on clouds and climate. This work describes a model to predict the CCN activity of organic compounds from functional group composition. Following previous methods in the literature, we test the ability of semi-empirical group contribution methods in Köhler theory to predict the effective hygroscopicity parameter, kappa. However, in our approach we also account for liquid–liquid phase boundaries to simulate phase-limited activation behavior. Model evaluation against a selected database of published laboratory measurements demonstrates that kappa can be predicted within a factor of 2. Simulation of homologous series is used to identify the relative effectiveness of different functional groups in increasing the CCN activity of weakly functionalized organic compounds. Hydroxyl, carboxyl, aldehyde, hydroperoxide, carbonyl, and ether moieties promote CCN activity while methylene and nitrate moieties inhibit CCN activity. The model can be incorporated into scale-bridging test beds such as the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to evaluate the evolution of kappa for a complex mix of organic compounds and to develop suitable parameterizations of CCN evolution for larger-scale models.

scholarly journals Prediction of cloud condensation nuclei activity for organic compounds using functional group contribution methods

2015 ◽  
Vol 8 (9) ◽  
pp. 7445-7475 ◽  
Author(s):  
M. D. Petters ◽  
S. M. Kreidenweis ◽  
P. J. Ziemann
Keyword(s):  
Organic Compounds ◽  
Field Experiments ◽  
Functional Group ◽  
Cloud Condensation Nuclei ◽  
Organic Aerosol ◽  
Group Contribution ◽  
Condensation Nuclei ◽  
Aerosol Composition ◽  
Group Contribution Methods ◽  
Ccn Activity

Abstract. A wealth of recent laboratory and field experiments demonstrate that organic aerosol composition evolves with time in the atmosphere, leading to changes in the influence of the organic fraction to cloud condensation nuclei (CCN) spectra. There is a need for tools that can realistically represent the evolution of CCN activity to better predict indirect effects of organic aerosol on clouds and climate. This work describes a model to predict the CCN activity of organic compounds from functional group composition. The model combines Köhler theory with semi-empirical group contribution methods to estimate molar volumes, activity coefficients and liquid-liquid phase boundaries to predict the effective hygroscopicity parameter, kappa. Model evaluation against a selected database of published laboratory measurements demonstrates that kappa can be predicted within a factor of two. Simulation of homologous series is used to identify the relative effectiveness of different functional groups in increasing the CCN activity of weakly functionalized organic compounds. Hydroxyl, carboxyl, aldehyde, hydroperoxide, carbonyl, and ether moieties promote CCN activity while methylene and nitrate moieties inhibit CCN activity. The model can be incorporated into scale-bridging testbeds such as the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere to evaluate the evolution of kappa for a complex mix of organic compounds and to develop suitable parameterizations of CCN evolution for larger scale models.

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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