How do organic vapors contribute to new-particle formation?

被引:97
作者
Donahue, Neil M. [1 ]
Ortega, Ismael K. [2 ]
Chuang, Wayne [1 ]
Riipinen, Ilona [1 ,2 ,3 ,4 ]
Riccobono, Francesco [6 ]
Schobesberger, Siegfried [2 ]
Dommen, Josef [6 ]
Baltensperger, Urs [6 ]
Kulmala, Markku [2 ]
Worsnop, Douglas R. [2 ,5 ]
Vehkamaki, Hanna [2 ]
机构
[1] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA
[2] Univ Helsinki, Dept Phys, Div Atmospher Sci, FI-00014 Helsinki, Finland
[3] Univ Stockholm, Dept Appl Environm Sci, Stockholm, Sweden
[4] Univ Stockholm, Bert Bolin Ctr Climate Res, Stockholm, Sweden
[5] Aerodyne Res Inc, Billerica, MA USA
[6] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland
基金
芬兰科学院; 瑞士国家科学基金会; 美国国家科学基金会; 瑞典研究理事会;
关键词
VOLATILITY BASIS-SET; ATMOSPHERIC SULFURIC-ACID; AEROSOL FORMATION; SECONDARY; NUCLEATION; GROWTH; CONDENSATION; OXIDATION; DILUTION; SIZE;
D O I
10.1039/c3fd00046j
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Highly oxidised organic vapors can effectively stabilize sulphuric acid in heteronuclear clusters and drive new-particle formation. We present quantum chemical calculations of cluster stability, showing that multifunctional species can stabilize sulphuric acid and also present additional polar functional groups for subsequent cluster growth. We also model the multi-generation oxidation of vapors associated with secondary organic aerosol formation using a two-dimensional volatility basis set. The steady-state saturation ratios and absolute concentrations of extremely low volatility products are sufficient to drive new-particle formation with sulphuric acid at atmospherically relevant rates.
引用
收藏
页码:91 / 104
页数:14
相关论文
共 56 条
[1]   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
[2]   How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation [J].
Bonn, B. ;
Kulmala, M. ;
Riipinen, I. ;
Sihto, S. -L. ;
Ruuskanen, T. M. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2008, 113 (D12)
[3]   Quantitative estimates of the volatility of ambient organic aerosol [J].
Cappa, C. D. ;
Jimenez, J. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (12) :5409-5424
[4]   Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer [J].
Chen, Modi ;
Titcombe, Mari ;
Jiang, Jingkun ;
Jen, Coty ;
Kuang, Chongai ;
Fischer, Marc L. ;
Eisele, Fred L. ;
Siepmann, J. Ilja ;
Hanson, David R. ;
Zhao, Jun ;
McMurry, Peter H. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (46) :18713-18718
[5]  
Dal Maso M, 2005, BOREAL ENVIRON RES, V10, P323
[6]   A two-dimensional volatility basis set - Part 2: Diagnostics of organic-aerosol evolution [J].
Donahue, N. M. ;
Kroll, J. H. ;
Pandis, S. N. ;
Robinson, A. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (02) :615-634
[7]   Theoretical constraints on pure vapor-pressure driven condensation of organics to ultrafine particles [J].
Donahue, N. M. ;
Trump, E. R. ;
Pierce, J. R. ;
Riipinen, I. .
GEOPHYSICAL RESEARCH LETTERS, 2011, 38
[8]   A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics [J].
Donahue, N. M. ;
Epstein, S. A. ;
Pandis, S. N. ;
Robinson, A. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (07) :3303-3318
[9]   Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions [J].
Donahue, Neil M. ;
Henry, Kaytlin M. ;
Mentel, Thomas F. ;
Kiendler-Scharr, Astrid ;
Spindler, Christian ;
Bohn, Birger ;
Brauers, Theo ;
Dorn, Hans P. ;
Fuchs, Hendrik ;
Tillmann, Ralf ;
Wahner, Andreas ;
Saathoff, Harald ;
Naumann, Karl-Heinz ;
Moehler, Ottmar ;
Leisner, Thomas ;
Mueller, Lars ;
Reinnig, Marc-Christopher ;
Hoffmann, Thorsten ;
Salo, Kent ;
Hallquist, Mattias ;
Frosch, Mia ;
Bilde, Merete ;
Tritscher, Torsten ;
Barmet, Peter ;
Praplan, Arnaud P. ;
DeCarlo, Peter F. ;
Dommen, Josef ;
Prevot, Andre S. H. ;
Baltensperger, Urs .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (34) :13503-13508
[10]   Coupled partitioning, dilution, and chemical aging of semivolatile organics [J].
Donahue, NM ;
Robinson, AL ;
Stanier, CO ;
Pandis, SN .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (08) :2635-2643