scholarly journals Ozone oxidation of oleic acid surface films decreases aerosol cloud condensation nuclei activity

2011 ◽  
Vol 116 (D16) ◽  
Author(s):  
A. N. Schwier ◽  
N. Sareen ◽  
T. L. Lathem ◽  
A. Nenes ◽  
V. F. McNeill

2017 ◽  
Vol 189 ◽  
pp. 69-81 ◽  
Author(s):  
Arindam Roy ◽  
Abhijit Chatterjee ◽  
Chirantan Sarkar ◽  
Sanat Kumar Das ◽  
Sanjay Kumar Ghosh ◽  
...  




2014 ◽  
Vol 14 (14) ◽  
pp. 7485-7497 ◽  
Author(s):  
B. Gantt ◽  
J. He ◽  
X. Zhang ◽  
Y. Zhang ◽  
A. Nenes

Abstract. One of the greatest sources of uncertainty in the science of anthropogenic climate change is from aerosol–cloud interactions. The activation of aerosols into cloud droplets is a direct microphysical linkage between aerosols and clouds; parameterizations of this process link aerosol with cloud condensation nuclei (CCN) and the resulting indirect effects. Small differences between parameterizations can have a large impact on the spatiotemporal distributions of activated aerosols and the resulting cloud properties. In this work, we incorporate a series of aerosol activation schemes into the Community Atmosphere Model version 5.1.1 within the Community Earth System Model version 1.0.5 (CESM/CAM5) which include factors such as insoluble aerosol adsorption and giant cloud condensation nuclei (CCN) activation kinetics to understand their individual impacts on global-scale cloud droplet number concentration (CDNC). Compared to the existing activation scheme in CESM/CAM5, this series of activation schemes increase the computation time by ~10% but leads to predicted CDNC in better agreement with satellite-derived/in situ values in many regions with high CDNC but in worse agreement for some regions with low CDNC. Large percentage changes in predicted CDNC occur over desert and oceanic regions, owing to the enhanced activation of dust from insoluble aerosol adsorption and reduced activation of sea spray aerosol after accounting for giant CCN activation kinetics. Comparison of CESM/CAM5 predictions against satellite-derived cloud optical thickness and liquid water path shows that the updated activation schemes generally improve the low biases. Globally, the incorporation of all updated schemes leads to an average increase in column CDNC of 150% and an increase (more negative) in shortwave cloud forcing of 12%. With the improvement of model-predicted CDNCs and better agreement with most satellite-derived cloud properties in many regions, the inclusion of these aerosol activation processes should result in better predictions of radiative forcing from aerosol–cloud interactions.



2019 ◽  
Author(s):  
Pascal Polonik ◽  
Christoph Knote ◽  
Tobias Zinner ◽  
Florian Ewald ◽  
Tobias Kölling ◽  
...  

Abstract. The realistic representation of cloud-aerosol interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon area has been one of the motivations for several field observations, including the airborne Aerosol, Cloud, Precipitation, and Radiation Interactions and DynamIcs of CONvective cloud systems – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA) campaign based in Manaus, Brazil in September 2014. In this work we combine in situ and remotely sensed aerosol, cloud, and atmospheric radiation data collected during ACRIDICON-CHUVA with regional, online-coupled chemistry-transport simulations to evaluate the model’s ability to represent the indirect effects of biomass burning aerosol on cloud microphysical properties (droplet number concentration and effective radius). We found agreement between modeled and observed median cloud droplet number concentrations (CDNC) for low values of CDNC, i.e., low levels of pollution. In general, a linear relationship between modeled and observed CDNC with a slope of two was found, which means a systematic underestimation of modeled CDNC as compared to measurements. Variability in cloud condensation nuclei (CCN) number concentrations and cloud droplet effective radii (reff) was also underestimated by the model. Modeled effective radius profiles began to saturate around 500 CCN per cm3 at cloud base, indicating an upper limit for the model sensitivity well below CCN concentrations reached during the burning season in the Amazon Basin. Regional background aerosol concentrations were sufficiently high such that the additional CCN emitted from local fires did not cause a notable change in modelled cloud microphysical properties. In addition, we evaluate a parameterization of CDNC at cloud base using more readily available cloud microphysical properties, aimed at in situ observations and satellite retrievals. Our study casts doubt on the validity of regional scale modeling studies of the cloud albedo effect in convective situations for polluted situations where the number concentration of CCN is greater than 500 cm−3.



2018 ◽  
Vol 18 (10) ◽  
pp. 7345-7359 ◽  
Author(s):  
Mingjin Wang ◽  
Tong Zhu ◽  
Defeng Zhao ◽  
Florian Rubach ◽  
Andreas Wahner ◽  
...  

Abstract. Condensation of carboxylic acids on mineral particles leads to coatings and impacts the particles' potential to act as cloud condensation nuclei (CCN). To determine how the CCN activity of mineral particles is impacted by carboxylic acid coatings, the CCN activities of CaCO3 particles and CaCO3 particles with oleic acid and malonic acid coatings were compared in this study. The results revealed that small amounts of oleic acid coating (volume fraction (vf) ≤4.3 %) decreased the CCN activity of CaCO3 particles, while more oleic acid coating (vf ≥16 %) increased the CCN activity of CaCO3 particles. This phenomenon has not been reported before. In contrast, the CCN activity of CaCO3 particles coated with malonic acid increased with the thickness of the malonic acid coating (vf =0.4–40 %). Even the smallest amounts of malonic acid coating (vf =0.4 %) significantly enhanced the CCN activity of CaCO3 particles from κ=0.0028±0.0001 to κ=0.0123±0.0005. This indicates that a small amount of water-soluble organic acid coating may significantly enhance the CCN activity of mineral particles. The presence of water vapor during the coating process with malonic acid additionally increased the CCN activity of the coated CaCO3 particles, probably because more CaCO3 reacts with malonic acid when sufficient water is available.



2020 ◽  
Vol 20 (3) ◽  
pp. 1591-1605 ◽  
Author(s):  
Pascal Polonik ◽  
Christoph Knote ◽  
Tobias Zinner ◽  
Florian Ewald ◽  
Tobias Kölling ◽  
...  

Abstract. The realistic representation of aerosol–cloud interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon region has been one of the motivations for several field campaigns, including the airborne “Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA)” campaign based in Manaus, Brazil, in September 2014. In this work we combine in situ and remotely sensed aerosol, cloud, and atmospheric radiation data collected during ACRIDICON-CHUVA with regional, online-coupled chemistry-transport simulations to evaluate the model's ability to represent the indirect effects of biomass burning aerosol on cloud microphysical and optical properties (droplet number concentration and effective radius). We found agreement between the modeled and observed median cloud droplet number concentration (CDNC) for low values of CDNC, i.e., low levels of pollution. In general, a linear relationship between modeled and observed CDNC with a slope of 0.3 was found, which implies a systematic underestimation of modeled CDNC when compared to measurements. Variability in cloud condensation nuclei (CCN) number concentrations was also underestimated, and cloud droplet effective radii (reff) were overestimated by the model. Modeled effective radius profiles began to saturate around 500 CCN cm−3 at cloud base, indicating an upper limit for the model sensitivity well below CCN concentrations reached during the burning season in the Amazon Basin. Additional CCN emitted from local fires did not cause a notable change in modeled cloud droplet effective radii. Finally, we also evaluate a parameterization of CDNC at cloud base using more readily available cloud microphysical properties, showing that we are able to derive CDNC at cloud base from cloud-side remote-sensing observations.



2015 ◽  
Vol 15 (21) ◽  
pp. 12211-12229 ◽  
Author(s):  
M. Paramonov ◽  
V.-M. Kerminen ◽  
M. Gysel ◽  
P. P. Aalto ◽  
M. O. Andreae ◽  
...  

Abstract. Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (NCCN) to the total number concentration of particles (NCN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations – exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A50 and A100, respectively) renders a much more stable dependence of A on S; A50 and A100 also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter κ decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations κ increased with size. In fact, in Hyytiälä, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5 % significance level. In a boreal environment the assumption of a size-independent κ can lead to a potentially substantial overestimation of NCCN at S levels above 0.6 %. The same is true for other locations where κ was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of NCCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol–cloud interactions in various environments.



2016 ◽  
Vol 113 (21) ◽  
pp. 5828-5834 ◽  
Author(s):  
Daniel Rosenfeld ◽  
Youtong Zheng ◽  
Eyal Hashimshoni ◽  
Mira L. Pöhlker ◽  
Anne Jefferson ◽  
...  

Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25° restricts the satellite coverage to ∼25% of the world area in a single day.



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