Organic Aerosol Growth Mechanisms and Their Climate-Forcing Implications

Surface- and volume-limited chemical reactions on and in atmospheric aerosol particles cause growth while changing organic composition by 13 to 24% per day. Many of these particles contain carbonaceous components from mineral dust and combustion emissions in Africa, Asia, and North America and reveal reaction rates that are three times slower than those typically used in climate models. These slower rates for converting from volatile or hydrophobic to condensed and hygroscopic organic compounds increase carbonaceous particle burdens in climate models by 70%, producing organic aerosol climate forcings of as much as –0.8 watt per square meter cooling and +0.3 watt per square meter warming.

[1]  A. R. Ravishankara,et al.  Heterogeneous and Multiphase Chemistry in the Troposphere , 1997 .

[2]  C. Liousse,et al.  Construction of a 1° × 1° fossil fuel emission data set for carbonaceous aerosol and implementation and radiative impact in the ECHAM4 model , 1999 .

[3]  S. Weiss,et al.  Chemical physics. Single-molecule spectroscopy comes of age. , 2001, Science.

[4]  Allen,et al.  Direct observation of heterogeneous chemistry in the atmosphere , 1998, Science.

[5]  M. Noguer,et al.  Climate change 2001: The scientific basis. Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change , 2002 .

[6]  David S. Covert,et al.  An exploration of aqueous oxalic acid production in the coastal marine atmosphere , 2004 .

[7]  J. Seinfeld,et al.  Reshaping the Theory of Cloud Formation , 2001, Science.

[8]  V. Grassian Heterogeneous uptake and reaction of nitrogen oxides and volatile organic compounds on the surface of atmospheric particles including oxides, carbonates, soot and mineral dust: Implications for the chemical balance of the troposphere , 2001 .

[9]  J. Penner,et al.  Large contribution of organic aerosols to cloud-condensation-nuclei concentrations , 1993, Nature.

[10]  A. Haines Climate change 2001: the scientific basis. Contribution of Working Group 1 to the Third Assessment report of the Intergovernmental Panel on Climate Change [Book review] , 2003 .

[11]  P. Crutzen,et al.  Human‐activity‐enhanced formation of organic aerosols by biogenic hydrocarbon oxidation , 2000 .

[12]  D. Koch Transport and direct radiative forcing of carbonaceous and sulfate aerosols in the GISS GCM , 2001 .