Kinetic equation of concurrent nucleation and chemical aging of an ensemble of aqueous organic aerosols.

Abstract

Using the formalism of classical nucleation theory, we derive a kinetic equation for the size and composition distribution of an ensemble of aqueous organic droplets evolving via nucleation and concomitant chemical aging. This distribution can be drastically affected by the enthalpy of heterogeneous chemical reactions and the depletion of organic trace gases absorbed by aerosols. A partial differential equation of second order for the temporal evolution of this distribution is obtained from the discrete equation of balance via Taylor series expansions. Once reduced to the canonical form of the multidimensional Fokker-Planck equation, this kinetic equation can be solved via the method of complete separation of variables. This kinetic equation opens a new direction in the development of the kinetic theory of first-order phase transitions, while its applications to the formation and evolution atmospheric organic aerosols via concurrent nucleation and chemical aging may drastically improve the accuracy of global climate models.