United States Environmental Protection Agency Environmental Sciences Research Laboratory Research Triangle Park NC 27711 * Research and Development EPA-600/S3-83-035 July 1983 Project Summary A Regional Scale Model (1000 km) of Photochemical Air Pollution: Part 1. Theoretical Formulation Robert G. Lamb A theoretical framework for a multi- day, 1000-km scale simulation model of photochemical oxidant is developed. It is structured in a highly modular form so that eventually the model can be applied through straightforward modifications to simulations of par- ticulates, visibility and acid rain. The model structure is based on phenomenological concepts and con- sists of three and one-half layers. The interface surfaces separating the layers are functions of both space and time that respond to variations in the mete- orological phenomena that each layer is intended to treat. Among the physi- cal and chemical processes affecting passage and distribution of photo- chemical concentrations that the model is designed to handle are: horizontal transport, photochemistry, nighttime wind shear and the nocturnal jet; cumulus cloud effects; mesoscale ver- tical motion; mesoscale eddy effects; terrain effects; subgrid scale chemis- try processes; natural sources of hy- drocarbons, NOX, and stratospheric ozone; and wet and dry removal pro- cesses, e.g., washout and deposition. The predictability of pollutant con- centrations at long range is considered, along with such related problems as the parameterization of "mesoscale" diffusion andthe design of model "vali- dation" experiments. A basis is estab- lished for estimating quantitatively the levels of uncertainty associated with dispersion model predictions. This report focuses on theoretical aspects of the model and the question of predictability. Results of the model's performance and quantitative assess- ments of its predictability will be pre- sented in subsequent parts of this report This Project Summary was developed by EPA's Environmental Sciences Re- search Laboratory, Research Triangle Park NC, to announce key findings of the research project that is fully doc- umented in a separate report of the same title (see Project Report ordering information at back). Introduction This project was begun in 1977 with the objective of developing a model for guiding the formulation of regional emis- sions control strategies. Initially the prin- cipal concern was with the photochemical oxidant; but in the course of its develop- ment, the model was constructed in a highly modular form that would allow straightforward applications to fine par- ticulates, visibility, and, possibly, acid deposition as well. When this project was begun, there did not exist an air pollution model that could simulate all the physical and chemical phenomena that are believed to control the fate of photochemical pollutants over large time and space domains. Among these phenomena are (not necessarily in order of importance): ' 1) Horizontal transport 2) Photochemistry, including the very slow reactions 3) Nighttime chemistry of the products and precursors of photochemical reactions ------- 4) Nighttime wind shear, stability stra- tification, and turbulence " episodes" associated with the nocturnal jet 5) Cumulus cloud effects. Venting pollutants from the mixed layer, perturbing photochemical reac- tions rates in the shadows, provid- ing sites for liquid phase reactions, influencing changes in the mixed layer depth, perturbing horizontal flow 6) Mesoscale eddy effects on urban plume trajectories and growth rates 7) Terrain effects on horizontal flows, removal, diffusion 8) Subgrid scale chemistry processes -- resulting from emissions from sources smaller than the model's grid can resolve 9) Natural sources of hydrocarbons, NOX, and stratospheric ozone 10) Wet and dry removal processes, e.g., washout and deposition A necessary condition for the credibility of a long range transport model is that all of these phenomena be taken into account, at least until it has been demonstrated that some of these processes play a negligible role. Of similar concern are several questions regarding fundamental aspects of modeling itself. Following are three questions that are relevant not only to the utility of pollution models in regulatory, decision- making roles, but also to the meaningful implementation of the model itself. (1) What aspects of pollutant concen- trations are models capable of pre- dicting? (2) Given our present state of knowledge, what are the theoretical limits on the accuracy with which these quantities can be predicted (assuming perfect emissions data chemical information, etc.)? (3) How does one assess the accuracy of a given model? These questions must be resolved before a model can be verified or used in any meaningful way. Procedure In order to design a viable model frame- work consistent with all the anticipated applications noted above, an attempt was made to derive from the observational evidence available at the time this program was initiated an estimate of the minimum vertical and horizontal resolutions neces- sary to describe regional scale air pollution phenomena. The aim was to arrive at the best compromise between the restrictions imposed upon the model by computer time and memory limitations and the need to describe as accurately as possible all of the important physical and chemical pro- cesses. The NO, 03, and meteorological data reported by the participants of the 1975 Northeast Oxidant Transport Study were analyzed and it was concluded that to describe the phenomena revealed by those data would require at the very least a three- level model: one level assigned to the surf ace layer, another layer assigned to the remainder of the daytime mixed layer, and an additional layer atop the mixed layer. The top level would be used in conjunction with the mixed layer to account for down- ward fluxes of stratospheric ozone as well as upward fluxes of ozone and its pre- cursors into the subsidence inversion layer above. Material that entered this top layer could be transported by winds aloft to areas outside the modeling region; it could reenter the mixed layer by subsidence or entrainment; it could enter precipitating clouds and be rained out of the atmosphere; or it could undergo chemical transforma- tion. Representing the subsidence inver- sion, where cumulus clouds often form under stagnant high pressure conditions, the top level of the model would be in- strumental in simulating the chemical sink effects of heterogeneous (within cloud droplets) reactions among ozone, its pre- cursors, and other natural and pollutant species. Including cloud effects in the model would be especially important in simulating S02 and sulfates. An extra "half layer" would be necessary adjacent to the ground to parameterize dry deposi- tion and subgrid scale chemistry processes induced by point and line sources of pollutants. Having three layers in a model is insuf- ficient in itself to simulate the phenomena we have discussed above. The need is, rather for three "dynamic" layers that are free to expand and contract locally in response to changes in the phenomena being modeled The model developed in this program possesses these properties. The surfaces that comprise the interfaces of adjacent layers are variable in both space and time in order that each layer can fully account for the changes that occur in its own domain of phenomena. Working in concert, the model's three and one-half layers can effect the simulation of all of the phenomena cited above. To address the questions of what models are capable of predicting, how accurately they can predict given variables and how one would proceed to verify the validity of a model, we considered the basic problem of model formulation from the viewpoint of fundamental mathematical principles. The aim was to delineate in mathematical terms the nature of the statements that one can deduce about natural phenomena, such as air pollutant concentrations, given descriptions of the universal laws govern- ing those phenomena and values of the parameters, in terms qf discrete observa- tions, involved in those laws. Conclusions Special numerical techniques were de- veloped to meet the rather unique needs of this model. One of these techniques is a high-order, explicit differencing scheme that suppresses errors in the advection and diffusion simulation that the nonlinear chemical processes would amplify. This scheme also permits the model domain to be handled in a piecewise fashion. Without this capability, awkward, inefficient com- puting procedures would be required to operate this large model on EPA's UNIVAC computer. Tests of this numerical method showed that its performance is superior in a number of important respects to that of existing alternative algorithms. Another special numerical technique developed for this project is a scheme that allows the set of nonlinear differential equations that describe air pollution chem- istry to be handled in their full form rather than in pseudosteady-state form. Coupling of the chemistry with the vertical fluxes of material among the model's three layers is accomplished with the aid of still another new algorithm that is computationally stable over virtually an infinite range of parameter values. Tests of these two numerical schemes showed that they provide an acceptable level of accuracy in much less computation time than alternative methods. The mathematical analyses of predicta- bility, model accuracy, and validation pro- cedures showed that physical laws anc discrete descriptions of atmospheric vari- ables are insufficient to define uniquely such variables as pollutant concentration distributions. As a consequence, even il all data used in the model were precise and the mathematical equations that describe the governing physical laws could be solvec exactly, a model still could not predict the concentration that would occur at a giver place at a given time. Rather, it coulc prescribe only a range of values in which the observed value would fall. Thus, the utility of a model in a given application is determined by the width of this interval o possible values. An ongoing aspect of this research program is to quantify the predic- tability of pollutant concentrations as £ function of averaging time, distance be- tween the source and receptor, the pol- ------- lutant species, meteorological conditions, and other relevant parameters. Results of this work will be presented in a future report. The EPA author Robert G. Lamb is with the Environmental Sciences Research Laboratory. Research Triangle Park, NC 27711. The complete report, entitled "A Regional Scale (1000 km) Model of Photo- chemical Air Pollution: Part 1. Theoretical Formulation," (Order No. PB 83-207 688; Cost: $20.50, subject to change) will be available only from: National Technical Information Service 5285 Port Royal Road Springfield. VA 22161 Telephone: 703-487-4650 The EPA author can be contacted at: Environmental Sciences Research Laboratory U.S. Environmental Protection Agency Research Triangle Park, NC 27711 ------- United States Environmental Protection Agency Center for Environmental Research Information Cincinnati OH 45268 Postage and Fees Paid Environmental Protection Agency EPA 335 Official Business Penalty for Private Use $300 PS 0000339 U S ENVIR PROTECTION AGENCY REGION 5 LIBRARY 230 S DEARBORN STREET CHICAGO IL 60604 ------- |