The dispersion of chemically reactive species in the atmospheric boundary layer

J. Vilà-Guerau de Arellano, A. Dosio, J. Vinuesa, A.A.M. Holtslag, S. Galmarini

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28 Citations (Scopus)

Abstract

The role of turbulence in the dispersion of atmospheric pollutants that react with linear (decay) and nonlinear (second-order) chemical reactions is examined. The most relevant processes that drive the reactivity of species emitted in a surface area or released by a point source are studied by deriving the dimensionless scaling numbers from equations for the atmospheric turbulent reacting flow. The first number is the ratio of the time scale of turbulence to the time scale of the chemical reaction, namely the Damkohler number. The second number is the ratio of the concentrations of the species present in the chemical transformations. In this paper, model results and experimental studies of turbulent reacting flows in the atmospheric boundary layer are presented to show the modifications and control exerted by turbulence on the atmospheric chemistry as a function of these numbers and processes. We also discuss how the chemical transformation is affected when species are in a state of chemical equilibrium. By studying the plume dispersion of a reactant, that decays with a simple chemical reaction, one can analyse the dependence of concentration fluctuations on the Damkohler number. The study is extended to plumes that react nonlinearly. In such reacting systems, the large gradients and segregation of species result in a significant reduction in the reaction rates. Because of this modification, the chemistry of species related to NOx and HOx can be very different from the chemistry in conditions where the species are uniformly mixed. The lack of complete observational evidence is hampering our understanding of these processes and our evaluation of numerical modelling results. Finally, we discuss briefly how to represent, in the form of a parameterization, the effect that turbulence can have on the reactivity of species emitted by a point source or an area source.
Original languageEnglish
Pages (from-to)23-38
JournalMeteorology and Atmospheric Physics
Volume87
Issue number1-3
DOIs
Publication statusPublished - 2004

Keywords

  • large-eddy simulation
  • surface-layer
  • concentration fluctuations
  • microscale turbulence
  • general-theory
  • fluxes
  • plume
  • chemistry
  • model
  • formulation

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