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Chemical Amplification (or Dampening) of the Twomey Effect: Conditions Derived from Droplet Activation Theory

T. A. RissmanDepartments of Chemical Engineering, and Environmental Science and Engineering, California Institute of Technology, Pasadena, California

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A. NenesDepartments of Chemical Engineering, and Environmental Science and Engineering, California Institute of Technology, Pasadena, California

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J. H. SeinfeldDepartments of Chemical Engineering, and Environmental Science and Engineering, California Institute of Technology, Pasadena, California

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Abstract

Cloud droplet number concentrations are controlled by both meteorological and microphysical factors. Microphysical factors include aerosol number concentration and composition. This paper examines the importance of microphysical phenomena compared to the sensitivity with respect to parcel updraft velocity in the activation of aerosols to become cloud droplets. Of the compositional (chemical) factors that can influence droplet number concentration, the effect of organics is examined through their ability to alter droplet surface tension and to contribute solute. A recent parameterization of aerosol activation (by Abdul-Razzak et al.) is extended to obtain analytical expressions for the sensitivity of activation to microphysical factors relative to updraft velocity. It is demonstrated that, under some conditions, the droplet number concentration can be as much as 1.5 times more sensitive to changes in aerosol composition than to updraft velocity. Chemical effects seem to be most influential for size distributions typical of marine conditions and decrease in importance for strongly anthropogenically perturbed conditions. The analysis indicates that the presence of surface-active species can lead to as much uncertainty as results from variations in updraft velocity. The presence of surfactant species also drastically changes the response of the cloud condensation nuclei to changes in the updraft velocity spectrum. Conditions are found under which an increase in dissolved organic compounds can actually lead to a decrease in cloud droplet number, a “contra-Twomey effect.” Results presented have more general implications than just for organic compounds and can apply, in principle, for any chemically induced activation effect.

Corresponding author address: Dr. J. H. Seinfeld, Departments of Chemical Engineering and Environmental Science and Engineering, CIT, Mail Code 210-41, Pasasdena, CA 91125. Email: seinfeld@caltech.edu

Abstract

Cloud droplet number concentrations are controlled by both meteorological and microphysical factors. Microphysical factors include aerosol number concentration and composition. This paper examines the importance of microphysical phenomena compared to the sensitivity with respect to parcel updraft velocity in the activation of aerosols to become cloud droplets. Of the compositional (chemical) factors that can influence droplet number concentration, the effect of organics is examined through their ability to alter droplet surface tension and to contribute solute. A recent parameterization of aerosol activation (by Abdul-Razzak et al.) is extended to obtain analytical expressions for the sensitivity of activation to microphysical factors relative to updraft velocity. It is demonstrated that, under some conditions, the droplet number concentration can be as much as 1.5 times more sensitive to changes in aerosol composition than to updraft velocity. Chemical effects seem to be most influential for size distributions typical of marine conditions and decrease in importance for strongly anthropogenically perturbed conditions. The analysis indicates that the presence of surface-active species can lead to as much uncertainty as results from variations in updraft velocity. The presence of surfactant species also drastically changes the response of the cloud condensation nuclei to changes in the updraft velocity spectrum. Conditions are found under which an increase in dissolved organic compounds can actually lead to a decrease in cloud droplet number, a “contra-Twomey effect.” Results presented have more general implications than just for organic compounds and can apply, in principle, for any chemically induced activation effect.

Corresponding author address: Dr. J. H. Seinfeld, Departments of Chemical Engineering and Environmental Science and Engineering, CIT, Mail Code 210-41, Pasasdena, CA 91125. Email: seinfeld@caltech.edu

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