In this paper variance spectra of chemically active species in a dry convective boundary layer are studied by means of large-eddy simulations (LESs). The aim is to quantify the impact of chemistry on the spatial fluctuations in the concentration fields. The computational domain has a large aspect ratio ( width/height 5 16) in order to encompass all relevant scales (mesoscale to microscale). Variance spectra are used to calculate a characteristic length scale of the species' concentration variability. By locating the peak in the spectrum, a "variance dominating length scale'' is derived. For a simple first-order reaction, this length scale demonstrates a clear dependence on the reaction rate: an increase in the reaction rate leads to a significant decrease of the length scale of the species. For a chemical cycle composed of a second-order reaction and first-order backreaction, the length scales turn out to depend much less on the reaction rate. The value of the length scales of the species involved appears to lie well in the mesoscale range, rather than the microscale range, demonstrating that concentration fluctuations are driven predominantly by scales much larger than the depth of the boundary layer. External perturbation of the chemical balance can have a direct impact on the variance spectra. For the case where a ( hypothetical) passing cloud switches off the chemical backreaction for a while, a dramatic drop in the length scale of the nonabundant species is observed. Once the feedback has been restored, a rapid increase of the length scale is observed. To better understand these results, a spectral model is developed that incorporates turbulent production and dissipation of variance, chemistry, and spectral transfer. The model gives valuable insight into the relative importance of these processes at each scale separately, and enables one to predict the value of the variance dominating length scale in the limiting cases of very slow and very fast chemistry.
|Journal||Journal of the Atmospheric Sciences|
|Publication status||Published - 2004|
- large-eddy simulation
- aircraft measurements