scholarly journals CCN closure study: Effects of aerosol chemical composition and mixing state

2015 ◽  
Vol 120 (2) ◽  
pp. 766-783 ◽  
Author(s):  
Deepika Bhattu ◽  
S. N. Tripathi
Keyword(s):  
Chemical Composition ◽  
Mixing State ◽  
Aerosol Chemical Composition

scholarly journals Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing

2018 ◽  
Vol 18 (9) ◽  
pp. 6907-6921 ◽  
Author(s):  
Jingye Ren ◽  
Fang Zhang ◽  
Yuying Wang ◽  
Don Collins ◽  
Xinxin Fan ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Black Carbon ◽  
Cloud Condensation Nuclei ◽  
Field Measurements ◽  
Minor Role ◽  
Mixing State ◽  
Mixing Processes ◽  
Size Dependent ◽  
Aerosol Mixing State ◽  
Aerosol Chemical Composition

Abstract. Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (NCCN). In this study, we predict NCCN under five assumed schemes of aerosol chemical composition and mixing state based on field measurements in Beijing during the winter of 2016. Our results show that the best closure is achieved with the assumption of size dependent chemical composition for which sulfate, nitrate, secondary organic aerosols, and aged black carbon are internally mixed with each other but externally mixed with primary organic aerosol and fresh black carbon (external–internal size-resolved, abbreviated as EI–SR scheme). The resulting ratios of predicted-to-measured NCCN (RCCN_p∕m) were 0.90 – 0.98 under both clean and polluted conditions. Assumption of an internal mixture and bulk chemical composition (INT–BK scheme) shows good closure with RCCN_p∕m of 1.0 –1.16 under clean conditions, implying that it is adequate for CCN prediction in continental clean regions. On polluted days, assuming the aerosol is internally mixed and has a chemical composition that is size dependent (INT–SR scheme) achieves better closure than the INT–BK scheme due to the heterogeneity and variation in particle composition at different sizes. The improved closure achieved using the EI–SR and INT–SR assumptions highlight the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. NCCN is significantly underestimated (with RCCN_p∕m of 0.66 – 0.75) when using the schemes of external mixtures with bulk (EXT–BK scheme) or size-resolved composition (EXT–SR scheme), implying that primary particles experience rapid aging and physical mixing processes in urban Beijing. However, our results show that the aerosol mixing state plays a minor role in CCN prediction when the κorg exceeds 0.1.

scholarly journals Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on filed measurement in Beijing

2017 ◽  
Author(s):  
Jingye Ren ◽  
Fang Zhang ◽  
Yuying Wang ◽  
Xinxin Fan ◽  
Xiaoai Jin ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Cloud Condensation Nuclei ◽  
Organic Aerosols ◽  
Minor Role ◽  
Mixing State ◽  
Mixing Processes ◽  
Kohler Theory ◽  
Bulk Chemical ◽  
A Minor ◽  
Aerosol Chemical Composition

Abstract. Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted area is crucial for determining CCN number concentrations (NCCN) accurately. In this study, we predict CCN number concentrations (NCCN) by applying κ-Köhler theory under five assumed schemes of aerosol chemical composition and mixing state based on field measurement in Beijing during the winter of 2016. Our results show that the EIS scheme (with an assumption that sulfate, nitrate, and secondary organic aerosols are internally mixed and that primary organic aerosols, POA, and black carbon, BC, are externally mixed; and the chemical composition is size dependent) achieves the best closure to predict NCCN with ratios of predicted-to-measured NCCN (RCCN_p/m) of 0.90–1.12 under both clean and polluted conditions over the campaign. Also, IB scheme (with an assumption of internal mixture and bulk chemical composition for particles) shows good closure with RCCN_p/m of 1.01–1.19 under clean conditions, implying that the IB assumption is sufficient for CCN prediction in continental clean regions. On polluted days, IS scheme (assuming particles with internal mixture and chemical composition is size-resolved) achieve better closure than the IB scheme due to the heterogeneity and variations in particle composition at different sizes. The improved closure achieved using EIS and IS assumptions highlights the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. NCCN is significantly underestimated (with RCCN_p/m of 0.6–0.8) by using the schemes of external mixture with bulk (EB) or size-resolved composition (ES), implying that the primary particles experience rapid aging and physical mixing processes in urban area. However, our results show that the mixing state of particles plays a minor role on CCN prediction when the κorg exceeds 0.1.

Aerosol chemical composition and light scattering during a winter season in Beijing

2015 ◽  
Vol 110 ◽  
pp. 36-44 ◽  
Author(s):  
Jun Tao ◽  
Leiming Zhang ◽  
Jian Gao ◽  
Han Wang ◽  
Faihe Chai ◽  
...  
Keyword(s):  
Light Scattering ◽  
Chemical Composition ◽  
Winter Season ◽  
Aerosol Chemical Composition

Aerosol chemical composition over Istanbul

2010 ◽  
Vol 408 (12) ◽  
pp. 2482-2491 ◽  
Author(s):  
C. Theodosi ◽  
U. Im ◽  
A. Bougiatioti ◽  
P. Zarmpas ◽  
O. Yenigun ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Aerosol Chemical Composition

scholarly journals Mixing state and compositional effects on CCN activity and droplet growth kinetics of size-resolved CCN in an urban environment

2012 ◽  
Vol 12 (21) ◽  
pp. 10239-10255 ◽  
Author(s):  
L. T. Padró ◽  
R. H. Moore ◽  
X. Zhang ◽  
N. Rastogi ◽  
R. J. Weber ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Water Soluble ◽  
Anthropogenic Sources ◽  
Droplet Growth ◽  
Mixing State ◽  
Aerosol Composition ◽  
Activation Kinetics ◽  
Aerosol Mixing State ◽  
Kinetics Of ◽  
Ccn Activity

Abstract. Aerosol composition and mixing state near anthropogenic sources can be highly variable and can challenge predictions of cloud condensation nuclei (CCN). The impacts of chemical composition on CCN activation kinetics is also an important, but largely unknown, aspect of cloud droplet formation. Towards this, we present in-situ size-resolved CCN measurements carried out during the 2008 summertime August Mini Intensive Gas and Aerosol Study (AMIGAS) campaign in Atlanta, GA. Aerosol chemical composition was measured by two particle-into-liquid samplers measuring water-soluble inorganic ions and total water-soluble organic carbon. Size-resolved CCN data were collected using the Scanning Mobility CCN Analysis (SMCA) method and were used to obtain characteristic aerosol hygroscopicity distributions, whose breadth reflects the aerosol compositional variability and mixing state. Knowledge of aerosol mixing state is important for accurate predictions of CCN concentrations and that the influence of an externally-mixed, CCN-active aerosol fraction varies with size from 31% for particle diameters less than 40 nm to 93% for accumulation mode aerosol during the day. Assuming size-dependent aerosol mixing state and size-invariant chemical composition decreases the average CCN concentration overprediction (for all but one mixing state and chemical composition scenario considered) from over 190–240% to less than 20%. CCN activity is parameterized using a single hygroscopicity parameter, κ, which averages to 0.16 ± 0.07 for 80 nm particles and exhibits considerable variability (from 0.03 to 0.48) throughout the study period. Particles in the 60–100 nm range exhibited similar hygroscopicity, with a κ range for 60 nm between 0.06–0.076 (mean of 0.18 ± 0.09). Smaller particles (40 nm) had on average greater κ, with a range of 0.20–0.92 (mean of 0.3 ± 0.12). Analysis of the droplet activation kinetics of the aerosol sampled suggests that most of the CCN activate as rapidly as calibration aerosol, suggesting that aerosol composition exhibits a minor (if any) impact on CCN activation kinetics.

scholarly journals Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques

2015 ◽  
Vol 15 (8) ◽  
pp. 4161-4178 ◽  
Author(s):  
A. Worringen ◽  
K. Kandler ◽  
N. Benker ◽  
T. Dirsch ◽  
S. Mertes ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Metal Oxides ◽  
Relative Number ◽  
Carbonaceous Material ◽  
Submicron Particles ◽  
Research Station ◽  
Mixing State ◽  
Separation Techniques ◽  
Potential Measurement ◽  
Virtual Impactor

Abstract. In the present work, three different techniques to separate ice-nucleating particles (INPs) as well as ice particle residuals (IPRs) from non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed-phase clouds and allow after evaporation in the instrument for the analysis of the residuals. The Fast Ice Nucleus Chamber (FINCH) coupled with the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated particles for analysis. The instruments were run during a joint field campaign which took place in January and February 2013 at the High Alpine Research Station Jungfraujoch (Switzerland). INPs and IPRs were analyzed offline by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine their size, chemical composition and mixing state. Online analysis of the size and chemical composition of INP activated in FINCH was performed by laser ablation mass spectrometry. With all three INP/IPR separation techniques high abundances (median 20–70%) of instrumental contamination artifacts were observed (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH + IN-PCVI: steel particles). After removal of the instrumental contamination particles, silicates, Ca-rich particles, carbonaceous material and metal oxides were the major INP/IPR particle types obtained by all three techniques. In addition, considerable amounts (median abundance mostly a few percent) of soluble material (e.g., sea salt, sulfates) were observed. As these soluble particles are often not expected to act as INP/IPR, we consider them as potential measurement artifacts. Minor types of INP/IPR include soot and Pb-bearing particles. The Pb-bearing particles are mainly present as an internal mixture with other particle types. Most samples showed a maximum of the INP/IPR size distribution at 200–400 nm in geometric diameter. In a few cases, a second supermicron maximum was identified. Soot/carbonaceous material and metal oxides were present mainly in the sub-micrometer range. Silicates and Ca-rich particles were mainly found with diameters above 1 μm (using ISI and FINCH), in contrast to the Ice-CVI which also sampled many submicron particles of both groups. Due to changing meteorological conditions, the INP/IPR composition was highly variable if different samples were compared. Thus, the observed discrepancies between the different separation techniques may partly result from the non-parallel sampling. The differences of the particle group relative number abundance as well as the mixing state of INP/IPR clearly demonstrate the need of further studies to better understand the influence of the separation techniques on the INP/IPR chemical composition. Also, it must be concluded that the abundance of contamination artifacts in the separated INP and IPR is generally large and should be corrected for, emphasizing the need for the accompanying chemical measurements. Thus, further work is needed to allow for routine operation of the three separation techniques investigated.

scholarly journals CCN activity of organic aerosols observed downwind of urban emissions during CARES

2013 ◽  
Vol 13 (4) ◽  
pp. 9355-9399 ◽  
Author(s):  
F. Mei ◽  
A. Setyan ◽  
Q. Zhang ◽  
J. Wang
Keyword(s):  
Chemical Composition ◽  
Water Solubility ◽  
Volume Fraction ◽  
Field Studies ◽  
High Water ◽  
Carbonaceous Aerosols ◽  
Mass Spectral ◽  
Least Squares Fit ◽  
The Relationship ◽  
Aerosol Chemical Composition

Abstract. During the Carbonaceous Aerosols and Radiative Effects Study (CARES), activation fraction of size-resolved aerosol particles and aerosol chemical composition were characterized at the T1 site (~60 km downwind of Sacramento, California) from 10 June to 28 June 2010. The hygroscopicity of CCN-active particles (κCCN) with diameter from 100 to 171 nm, derived from the size-resolved activated fraction, varied from 0.10 to 0.21, with an average of 0.15, which was substantially lower than that proposed for continental sites in earlier studies. The low κCCN value was due to the high organic volume fraction, averaged over 80% at the T1 site. The derived κCCN exhibited little diurnal variation, consistent with the relatively constant organic volume fraction observed. At any time, over 90% of the size selected particles with diameter between 100 and 171 nm were CCN active, suggesting most particles within this size range were aged background particles. Due to the large organic volume fraction, organic hygroscopicity (κorg) strongly impacted particle hygroscopicity and therefore calculated CCN concentration. For vast majority of the cases, an increase of κorg from 0.03 to 0.18, which are within the typical range, doubled the calculated CCN concentration. Organic hygroscopicity was derived from κCCN and aerosol chemical composition, and its variations with the fraction of total organic mass spectral signal at m/z 44 (f44) and O : C were compared to results from previous studies. Overall, the relationships between κorg and f44 are quite consistent for organic aerosol (OA) observed during field studies and those formed in smog chamber. Compared to the relationship between κorg and f44, the relationship between κorg and O : C exhibits more significant differences among different studies, suggesting κorg may be better parameterized using f44. A least squares fit yielded κorg = 2.04 (± 0.07) × f44 − 0.11 (± 0.01) with the Pearson R2 value of 0.71. One possible explanation for the stronger correlation between κorg and f44 is that the m/z 44 signal (mostly contributed by the CO2+ ion) is more closely related to organic acids, which may dominate the overall κorg due to their relatively high water solubility and hygroscopicity.

Sign in / Sign up

Export Citation Format

Share Document