Multi-scale Atmospheric Dispersion Modelling by Use of Adaptive Gridding Techniques

An accurate prediction of the transport-reaction behaviour of atmospheric chemical species is required to fully understand the impact on the environment of pollution emissions. Elevated levels of secondary pollutants such as ozone in the lower atmosphere can be harmful to the health of both plants and animals, and can cause damage to property present in the urban environment. Detailed models of pollution mechanisms must therefore be developed through comparisons with field measurements to aid the selection of effective abatement policies. Such models must satisfy accuracy requirements both in terms of the number of species represented, and the spatial resolution of species profiles. Computational expense often compels current models to sacrifice detail in one of these areas. This paper attempts to address the latter point by presenting an atmospheric transport-reaction modelling strategy based upon a finite volume discretisation of the atmospheric dispersion equation. The source terms within this equation are provided by an appropriate reduced chemical scheme modelling the major species in the boundary layer. Reaction and transport discretisations are solved efficiently via a splitting technique applied at the level of the non-linear equations. The solution grid is generated using time dependant adaptive techniques, which provide a finer grid around regions of high spatial error in order to adequately resolve species concentration profiles. The techniques discussed are applied in two dimensions employing emissions from both point and area sources. Preliminary results show that the application of adaptive gridding techniques to atmospheric dynamics modelling can provide more accurately resolved species concentration profiles, accompanied by a reduced CPU time invested in solution. Such a model will provide the basis for high resolution studies of the multiple scale interactions between spatially inhomogeneous source patterns in urban and regional environments.     

Observations of urban airborne particle number concentrations during rush-hour conditions: analysis of the number based size distributions and modal parameters

A summertime study of the number concentration and the size distribution of combustion derived nanometre sized particles (termed nanoparticles) from diesel and spark-ignition (SI) engine emissions were made under rush-hour and free-flow traffic conditions at an urban roadside location in Leeds, UK in July 2003. The measured total particle number concentrations (N(TOTAL)) were of the order 1.8 x 10(4) to 3.4 x 10(4) cm(-3), and tended to follow the diurnal traffic flow patterns. The N(TOTAL) was dominated by particles < or =100 nm in diameter which accounted for between 89-93% of the measured particle number. By use of a log-normal fitting procedure, the modal parameters of the number based particle size distribution of urban airborne particulates were derived from the roadside measurements. Four component modes were identified. Two nucleation modes were found, with a smaller, more minor, mode composed principally of sub-11 nm particles, believed to be derived from particles formed from the nucleation of gaseous species in the atmosphere. A second mode, much larger in terms of number, was composed of particles within the size range of 10-20 nm. This second mode was believed to be principally derived from the condensation of the unburned fuel and lube oil (the solvent organic fraction or SOF) as it cooled on leaving the engine exhaust. Third and fourth modes were noted within the size ranges of 28-65 nm and 100-160 nm, respectively. The third mode was believed to be representative of internally mixed Aitken mode particles composed of a soot/ash core with an adsorbed layer of readily volatilisable material. The fourth mode was believed to be composed of chemically aged, secondary particles. The larger nucleation and Aitken modes accounted for between 80-90% of the measured N(TOTAL), and the particles in these modes were believed to be derived from SI and diesel engine emissions. The overall size distribution, particularly in modes II-IV, was observed to be strongly related to the number of primary particle emissions, with larger count median diameters observed under conditions where low numbers of primary soot based particles were present.     

The effects of parametric uncertainties in simulations of a reactive plume using a Lagrangian stochastic model

A combined Lagrangian stochastic model with micro-mixing and chemical sub-models is used to investigate a reactive plume of nitrogen oxides (NO_x) released into a turbulent grid flow doped with ozone (O₃). Sensitivities to the model input parameters are explored for different source NO_x scenarios. The wind tunnel experiments of Brown and Bilger (1996) provide the simulation conditions for the first case study where photolysis reactions are not included and the main uncertainties occur in parameters defining the turbulence scales, source size and reaction rate of NO with O₃. Using nominal values of the parameters from previous studies, the model gives a good representation of the radial profile of the conserved mean scalar ${\overline{\Gamma }}_{{\text{NO}}_{\text{x}}}$ although slightly over predicts peak mean NO₂ concentrations ${\overline{\Gamma }}_{{\text{NO}}_{\text{2}}}$ compared to the experiments. The high dimensional model representation (HDMR) method is used to investigate the effects of uncertainties in model inputs on the simulation of chemical species concentrations. For this scenario, the Lagrangian velocity structure function coefficient has the largest impact on simulated ${\overline{\Gamma }}_{{\text{NO}}_{\text{x}}}$ profiles. Photolysis reactions are then included in a chemical scheme consisting of eight reactions between species NO, O, O₃ and NO₂. Independent and interactive effects of 22 input parameters are studied for two source NO_x scenarios using HDMR, including turbulence parameters, temperature dependant rate parameters, photolysis rates, temperature, fraction of NO in total NO_x at the source and background ozone concentration [O₃]. For this reactive case, the variance in the predicted mean plume centre ${\overline{\Gamma }}_{{\text{O}}_{\text{3}}}$ is caused by parameters describing both physical (mixing time-scale coefficient) and chemical processes (activation energy for the reaction O₃+NO). The variance in predicted plume centre ${\overline{\Gamma }}_{{\text{NO}}_{\text{2}}}$ and root mean square NO₂ concentration ${\gamma }_{{\text{NO}}_{\text{2}}}^{\prime }$, is strongly influenced by the fraction of NO in the source NO_x, and to a lesser extent the mixing time-scale coefficient. Adjusting the latter gives improved agreement with the Brown and Bilger experiment. Some weak parameter interactions are observed.