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

被引:65
作者
Bhattu, Deepika [1 ]
Tripathi, S. N. [1 ,2 ]
机构
[1] Indian Inst Technol Kanpur, Dept Civil Engn, Kanpur, Uttar Pradesh, India
[2] Indian Inst Technol Kanpur, Ctr Environm Sci & Engn, Kanpur, Uttar Pradesh, India
关键词
closure; hygroscopicity; organics; O:C ratio; CCN prediction; CLOUD-CONDENSATION-NUCLEI; SECONDARY ORGANIC AEROSOL; SIZE-RESOLVED MEASUREMENTS; BIOMASS BURNING SMOKE; MASS-SPECTROMETER; HIGH-RESOLUTION; PART; ATMOSPHERIC AEROSOLS; SOURCE APPORTIONMENT; DROPLET GROWTH;
D O I
10.1002/2014JD021978
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
This study presents a detailed cloud condensation nuclei (CCN) closure study that investigates the effects of chemical composition (bulk and size resolved) and mixing state (internal and external) on CCN activity of aerosols. Measurements of the chemical composition, aerosol size distribution, total number concentration, and CCN concentration at supersaturation (SS = 0.2-1.0%) were performed during the winter season in Kanpur, India. Among the two cases considered here, better closure results are obtained for case 1 (low total aerosol loading, 49.54 26.42 g m(-3), and high O:C ratio, 0.61 0.07) compared to case 2 (high total aerosol loading, 101.05 18.73 g m(-3), and low O:C ratio, 0.42 0.06), with a maximum reduction of 3-81% in CCN overprediction for all depleted SS values (0.18-0.60%). Including the assumption that less volatile oxidized organic aerosols represent the soluble organic fraction reduced the overprediction to at most 40% and 129% in the internal and external mixing scenarios, respectively. At higher depleted SS values (0.34-0.60%), size-resolved chemical composition with an internal mixing state performed well in CCN closure among all organic solubility scenarios. However, at a lower depleted SS value (0.18%), closure is found to be more sensitive to both the chemical composition and mixing state of aerosols. At higher SS values, information on the solubility of organics and size-resolved chemical composition is required for accurate CCN predictions, whereas at lower SS values, information on the mixing state in addition to the solubility of organics and size-resolved chemical composition is required. Overall, (total) values are observed to be independent of the O:C ratio [(total)= (0.36 +/- 0.01) x O:C - (0.03 +/- 0.01)] in the range of 0.2<O:C<0.81, which indicates that the variation in the chemical composition of aerosols is not well represented by the changes in the O:C ratio alone.
引用
收藏
页码:766 / 783
页数:18
相关论文
共 80 条
[1]   Carbonaceous and inorganic composition in long-range transported aerosols over northern Japan: Implication for aging of water-soluble organic fraction [J].
Aggarwal, Shankar Gopala ;
Kawamura, Kimitaka .
ATMOSPHERIC ENVIRONMENT, 2009, 43 (16) :2532-2540
[2]   Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) - Part 1: Fine particle composition and organic source apportionment [J].
Aiken, A. C. ;
Salcedo, D. ;
Cubison, M. J. ;
Huffman, J. A. ;
DeCarlo, P. F. ;
Ulbrich, I. M. ;
Docherty, K. S. ;
Sueper, D. ;
Kimmel, J. R. ;
Worsnop, D. R. ;
Trimborn, A. ;
Northway, M. ;
Stone, E. A. ;
Schauer, J. J. ;
Volkamer, R. M. ;
Fortner, E. ;
de Foy, B. ;
Wang, J. ;
Laskin, A. ;
Shutthanandan, V. ;
Zheng, J. ;
Zhang, R. ;
Gaffney, J. ;
Marley, N. A. ;
Paredes-Miranda, G. ;
Arnott, W. P. ;
Molina, L. T. ;
Sosa, G. ;
Jimenez, J. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (17) :6633-6653
[3]   O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry [J].
Aiken, Allison C. ;
Decarlo, Peter F. ;
Kroll, Jesse H. ;
Worsnop, Douglas R. ;
Huffman, J. Alex ;
Docherty, Kenneth S. ;
Ulbrich, Ingrid M. ;
Mohr, Claudia ;
Kimmel, Joel R. ;
Sueper, Donna ;
Sun, Yele ;
Zhang, Qi ;
Trimborn, Achim ;
Northway, Megan ;
Ziemann, Paul J. ;
Canagaratna, Manjula R. ;
Onasch, Timothy B. ;
Alfarra, M. Rami ;
Prevot, Andre S. H. ;
Dommen, Josef ;
Duplissy, Jonathan ;
Metzger, Axel ;
Baltensperger, Urs ;
Jimenez, Jose L. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (12) :4478-4485
[4]   Elemental analysis of organic species with electron ionization high-resolution mass spectrometry [J].
Aiken, Allison. C. ;
DeCarlo, Peter F. ;
Jimenez, Jose L. .
ANALYTICAL CHEMISTRY, 2007, 79 (21) :8350-8358
[5]  
[Anonymous], 2007 ANN C AM ASS AE
[6]   Airborne cloud condensation nuclei measurements during the 2006 Texas Air Quality Study [J].
Asa-Awuku, Akua ;
Moore, Richard H. ;
Nenes, Athanasios ;
Bahreini, Roya ;
Holloway, John S. ;
Brock, Charles A. ;
Middlebrook, Ann M. ;
Ryerson, Thomas B. ;
Jimenez, Jose L. ;
DeCarlo, Peter F. ;
Hecobian, Arsineh ;
Weber, Rodney J. ;
Stickel, Robert ;
Tanner, Dave J. ;
Huey, Lewis G. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2011, 116
[7]   Inter-seasonal variability in size-resolved CCN properties at Kanpur, India [J].
Bhattu, Deepika ;
Tripathi, Sachchida Nand .
ATMOSPHERIC ENVIRONMENT, 2014, 85 :161-168
[8]   Closure between measured and modeled cloud condensation nuclei (CCN) using size-resolved aerosol compositions in downtown Toronto [J].
Broekhuizen, K. ;
Chang, R. Y. -W. ;
Leaitch, W. R. ;
Li, S. -M. ;
Abbatt, J. P. D. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2006, 6 :2513-2524
[9]   Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer [J].
Canagaratna, M. R. ;
Jayne, J. T. ;
Jimenez, J. L. ;
Allan, J. D. ;
Alfarra, M. R. ;
Zhang, Q. ;
Onasch, T. B. ;
Drewnick, F. ;
Coe, H. ;
Middlebrook, A. ;
Delia, A. ;
Williams, L. R. ;
Trimborn, A. M. ;
Northway, M. J. ;
DeCarlo, P. F. ;
Kolb, C. E. ;
Davidovits, P. ;
Worsnop, D. R. .
MASS SPECTROMETRY REVIEWS, 2007, 26 (02) :185-222
[10]   Hygroscopicity of water-soluble organic compounds in atmospheric aerosols: Amino acids and biomass burning derived organic species [J].
Chan, MN ;
Choi, MY ;
Ng, NL ;
Chan, CK .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (06) :1555-1562