scholarly journals Cloud condensation nuclei prediction error from application of Köhler theory: Importance for the aerosol indirect effect

2007 ◽  
Vol 112 (D12) ◽  
Author(s):  
Rafaella-Eleni P. Sotiropoulou ◽  
Athanasios Nenes ◽  
Peter J. Adams ◽  
John H. Seinfeld
Keyword(s):  
Indirect Effect ◽  
Prediction Error ◽  
Cloud Condensation Nuclei ◽  
Condensation Nuclei ◽  
Aerosol Indirect Effect ◽  
Kohler Theory

scholarly journals Weak global sensitivity of cloud condensation nuclei and the aerosol indirect effect to Criegee + SO<sub>2</sub> chemistry

2013 ◽  
Vol 13 (6) ◽  
pp. 3163-3176 ◽  
Author(s):  
J. R. Pierce ◽  
M. J. Evans ◽  
C. E. Scott ◽  
S. D. D'Andrea ◽  
D. K. Farmer ◽  
...  
Keyword(s):  
Boundary Layers ◽  
Indirect Effect ◽  
Cloud Condensation Nuclei ◽  
Chemical Mechanism ◽  
Model Parameters ◽  
Condensation Nuclei ◽  
Aerosol Indirect Effect ◽  
Global Sensitivity ◽  
Cloud Albedo ◽  
The Impact

Abstract. H2SO4 vapor is important for the nucleation of atmospheric aerosols and the growth of ultrafine particles to cloud condensation nuclei (CCN) sizes with important roles in the global aerosol budget and hence planetary radiative forcing. Recent studies have found that reactions of stabilized Criegee intermediates (CIs, formed from the ozonolysis of alkenes) with SO2 may be an important source of H2SO4 that has been missing from atmospheric aerosol models. For the first time in a global model, we investigate the impact of this new source of H2SO4 in the atmosphere. We use the chemical transport model, GEOS-Chem, with the online aerosol microphysics module, TOMAS, to estimate the possible impact of CIs on present-day H2SO4, CCN, and the cloud-albedo aerosol indirect effect (AIE). We extend the standard GEOS-Chem chemistry with CI-forming reactions (ozonolysis of isoprene, methyl vinyl ketone, methacrolein, propene, and monoterpenes) from the Master Chemical Mechanism. Using a fast rate constant for CI+SO2, we find that the addition of this chemistry increases the global production of H2SO4 by 4%. H2SO4 concentrations increase by over 100% in forested tropical boundary layers and by over 10–25% in forested NH boundary layers (up to 100% in July) due to CI+SO2 chemistry, but the change is generally negligible elsewhere. The predicted changes in CCN were strongly dampened to the CI+SO2 changes in H2SO4 in some regions: less than 15% in tropical forests and less than 2% in most mid-latitude locations. The global-mean CCN change was less than 1% both in the boundary layer and the free troposphere. The associated cloud-albedo AIE change was less than 0.03 W m−2. The model global sensitivity of CCN and the AIE to CI+SO2 chemistry is significantly (approximately one order-of-magnitude) smaller than the sensitivity of CCN and AIE to other uncertain model inputs, such as nucleation mechanisms, primary emissions, SOA (secondary organic aerosol) and deposition. Similarly, comparisons to size-distribution measurements show that uncertainties in other model parameters dominate model biases in the model-predicted size distributions. We conclude that improvement in the modeled CI+SO2 chemistry would not likely lead to significant improvements in present-day CCN and AIE predictions.

scholarly journals Global cloud condensation nuclei influenced by carbonaceous combustion aerosol

2011 ◽  
Vol 11 (3) ◽  
pp. 6999-7044 ◽  
Author(s):  
D. V. Spracklen ◽  
K. S. Carslaw ◽  
U. Pöschl ◽  
A. Rap ◽  
P. M. Forster
Keyword(s):  
Black Carbon ◽  
Carbon Emissions ◽  
Indirect Effect ◽  
Cloud Condensation Nuclei ◽  
Pollution Sources ◽  
Condensation Nuclei ◽  
Aerosol Indirect Effect ◽  
Aerosol Model ◽  
Cloud Albedo ◽  
Global Mean

Abstract. Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (particles upon which cloud drops form) so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to cloud drops has not been evaluated on the global scale. By combining extensive observations of cloud condensation nuclei concentrations and a global aerosol model, we show that carbonaceous combustion aerosol accounts for more than half of global cloud condensation nuclei. The evaluated model predicts that wildfire and pollution (fossil fuel and biofuel) carbonaceous combustion aerosol causes a global mean aerosol indirect effect of −0.34 W m−2 due to changes in cloud albedo, with pollution sources alone causing a global mean aerosol indirect effect of −0.23 W m−2. The small size of carbonaceous combustion particles from pollution sources means that whilst they account for only one-third of the emitted mass from these sources they cause two-thirds of the cloud albedo indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for to ensure that black carbon emissions controls that reduce the high number concentrations of small pollution particles have the desired net effect on climate.

scholarly journals Weak sensitivity of cloud condensation nuclei and the aerosol indirect effect to Criegee + SO<sub>2</sub> chemistry

2012 ◽  
Vol 12 (12) ◽  
pp. 33127-33163 ◽  
Author(s):  
J. R. Pierce ◽  
M. J. Evans ◽  
C. E. Scott ◽  
S. D. D'Andrea ◽  
D. K. Farmer ◽  
...  
Keyword(s):  
Boundary Layers ◽  
Indirect Effect ◽  
Ultrafine Particles ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Chemical Mechanism ◽  
Model Parameters ◽  
Condensation Nuclei ◽  
Aerosol Indirect Effect ◽  
Cloud Albedo

Abstract. H2SO4 vapor is important for the nucleation of atmospheric aerosols and the growth of ultrafine particles to cloud condensation nuclei (CCN) sizes. Recent studies have found that reactions of stabilized Criegee intermediates (CIs, formed from the ozonolysis of alkenes) with SO2 may be an important source of H2SO4 that has been missing from atmospheric aerosol models. In this paper, we use the chemical transport model, GEOS-Chem, with the online aerosol microphysics module, TOMAS, to estimate the possible impact of CIs on present-day H2SO4, CCN, and the cloud-albedo aerosol indirect effect (AIE). We extend the standard GEOS-Chem chemistry with CI-forming reactions (ozonolysis of isoprene, methyl vinyl ketone, methacrolein, propene, and monoterpenes) from the Master Chemical Mechanism. Using a fast rate constant for CI+SO2, we find that the addition of this chemistry increases the global production of H2SO4 by 4%. H2SO4 concentrations increase by over 100% in forested tropical boundary layers and by over 10–25% in forested NH boundary layers (up to 100% in July) due to CI + SO2 chemistry, but the change is generally negligible elsewhere. The predicted changed in CCN were strongly dampened to the CI + SO2 changes in H2SO4 in these regions: less than 15% in tropical forests and less than 2% in most mid-latitude locations. The global-mean CCN change was less than 1% both in the boundary layer and the free troposphere. The associated cloud-albedo AIE change was less than 0.03 W m−2. The model global sensitivity of CCN and the AIE to CI + SO2 chemistry is significantly (approximately one order-of-magnitude) smaller than the sensitivity of CCN and AIE to other uncertain model inputs, such as nucleation mechanisms, primary emissions, SOA and deposition. Similarly, comparisons to size-distribution measurements show that uncertainties in other model parameters dominate model biases in the model-predicted size distributions. We conclude that improvement in the modeled CI + SO2 chemistry would not likely to lead to significant improvements in present-day CCN and AIE predictions.

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 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 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 Exploring the First Aerosol Indirect Effect over the Maritime Continent Using a Ten-Year Collocated MODIS, CALIOP, and Model Dataset

2018 ◽  
Author(s):  
Alexa D. Ross ◽  
Robert E. Holz ◽  
Gregory Quinn ◽  
Jeffrey S. Reid ◽  
Peng Xian ◽  
...  
Keyword(s):  
Indirect Effect ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Effective Radius ◽  
Satellite Observations ◽  
Orthogonal Polarization ◽  
High Background ◽  
Aerosol Indirect Effect ◽  
Moderate Resolution Imaging Spectroradiometer ◽  
Complex Relationships

Abstract. Satellite observations and model simulations cannot, by themselves, give full insight into the complex relationships between aerosols and clouds. This is especially the case over the greater Southeast Asia, an area that is particularly sensitive to changes in precipitation yet possesses some of the world’s largest observability and predictability challenges. We present a new collocated dataset that combines satellite observations from Aqua's Moderate-resolution Imaging Spectroradiometer (MODIS) and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) with the Navy Aerosol Analysis and Prediction System (NAAPS). The dataset is designed with the capability to investigate aerosol-cloud relationships and provides coincident and vertically resolved cloud and aerosol observations for a ten-year period. Using model reanalysis aerosol fields from the NAAPS and coincident cloud liquid effective radius retrievals from MODIS (removing cirrus contamination using CALIOP), we investigate the first aerosol indirect effect. We find overall that as expected, aerosol loading anti-correlates with cloud effective radius, with maximum sensitivity in cumulous mediocris clouds with heights in the 3–4.5 km level. The highest susceptibility in droplet effective radius to modeled perturbations in particle concentrations were found in the more remote regions of the western Pacific Ocean and Indian Ocean. Conversely, there was much less variability in cloud droplet size near emission sources over both land and water. We hypothesize this is suggestive of a high background aerosol population already saturating the cloud condensation nuclei budget.

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